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an endogenous inhibitor of granzyme B (GzmB)
has emerged as a critical factor in the resistance to immunotherapy by protecting cancer cells from GzmB-induced cytotoxicity
its role in chemosensitivity remains unknown
we show that gemcitabine (GEM) treatment upregulates SERPINB9 through transcription factor ATF-3
GEM also induces the expression of GzmB and knockout or knockdown of SERPINB9 results in enhanced response of tumor cells to GEM
suggesting a role of GzmB/SERPINB9 axis in regulating chemosensitivity
To facilitate the therapeutic translation of these findings
we engineer POEM nanocarrier (consisting of lipid-derivatized polylysine (PEG-PLL-Oleic acid
and GEM-conjugated polylysine (PEG-PLL-OA-GEM
PPO/PPOGEM (POEM)) that is highly effective in codelivery of built-in GEM and loaded SERPINB9 short interfering RNA (siSPB9)
GEM conjugation introduces an additional mechanism of carrier/siRNA interaction in addition to charge-mediated interaction and enables efficient i.v
we show that co-delivery of GEM and siSPB9 significantly improves antitumor efficacy and remodels the tumor immune microenvironment in pancreatic cancer models
supporting a promising therapeutic strategy
selective inhibition of SPB9 activity in tumor cells and immunosuppressive immune cells while preserving its function in CTLs shall represent an attractive and effective strategy to boost ICB as well as other immunotherapies
the specific role of SPB9 in modulating the response of cancer cells to chemotherapeutic agents remains poorly understood
we show that GEM also induces SPB9 expression in tumor cells or tissues in vitro and in vivo
suggesting another feedback mechanism that negatively regulates the antitumor immune response
We study the mechanism by which GEM induces the SPB9 gene expression at transcriptional level
We further evaluate the role of GzmB/SPB9 axis in regulating the chemosensitivity of PCa cells to GEM
POEM (PPO/PPOGEM) nanocarrier is developed and evaluated for codelivery of GEM and siSPB9 to overcome both chemotherapy and immune resistance
The broad implications of these findings in cancer chemotherapy require more studies in the future
our data suggests that SPB9 KD or inhibition in tumor cells may benefit increased sensitivity to GEM-based chemotherapy in addition to its benefits in improving antitumor immune response
a PPO with a PEG/OA ratio of 5:2 and without further amino acid modification formed the most effective siRNA NPs with PPOGEM in terms of the amounts of Cy5.5 signals in the tumor tissues
as well as the ratios of the signals in tumors over those in other normal tissues/organs
This PPO was selected for further optimization of POEM/siRNA via extensive characterizations of the biophysical properties and in vivo distribution of 18 NPs that vary in PPOGEM/PPO/siRNA ratio
indicating that PPOGEM helps stabilize the system
siRNA was well loaded into POEM NPs at an N/P ratio of 5/1
Increasing the amounts of PPOGEM led to a gradual decrease of zeta potential likely due to the shielding effect from PPOGEM
at an N/P ratio of 5/1 and a PPOGEM/siRNA mass ratio of 50/1
the POEM/siRNA system demonstrated the most desirable biophysical properties with a size of ~45.6 nm and a zeta potential of around 9.3 mV (NPs with zeta potential in a range of −10 to +10 are considered close to neutral)
the zeta potential of the NPs could not be reduced to below 10 mV at all PPO/Psugar ratios examined
These data highlight the significant role of GEM in formulating the POEM NP system
it is obvious that the POEM system (blue curve
~54.87 Å) exhibits lower RoG values than the control polymer (red curve
This can be further explained by the representative conformation of POEM/siRNA
displayed at the bottom right of the panel
where siRNA effectively interacts with PPOGEM through both T-shaped π-π and hydrogen bonding interactions
It is emphasized that during the simulation
the whole NP system was constructed based on a molar ratio of PPOGEM (or Psugar)
the simulation accurately represents the composition of the NPs
NPs are composed of numerous copies of the simulation system
While the RoG difference between the POEM and Psugar systems is only around 1 Å in the simulation
this small difference at the unit level can lead to a significant variation in the overall size of the assembled NPs
the POEM system (~40 nm) and the Psugar system (~160 nm) exhibit a substantial difference in their final dimensions
The in vitro gene knockdown efficiency of POEM NPs was evaluated using KPC-C2-Luc and Panc02-Luc cell lines (Supplementary Fig. 12)
POEM NPs were more effective than the commercial siRNA transfection reagent RNAiMAX in mediating the siLuc transfection and silencing luciferase transgene expression in both cell lines
The long circulation time of POEM/siRNA is likely attributed to the excellent stability of the NPs in blood
which contributes to the effective tumor targeting
clearly demonstrating the therapeutic benefit of codelivery of gemcitabine and siSPB9 using POEM NPs
These findings underscore the excellent safety profile of co-delivery of siSPB9 and GEM using POEM NPs
at dosages that have shown significant therapeutic efficacy
These results suggest that the combination of POEM/siSPB9 with anti-PD-1 treatment represents a promising regimen towards GEM resistant pancreatic cancer
Our data suggests that KD of SPB9 can directly sensitize PCa to GEM treatment in addition to improving the antitumor immune response
It remains to be studied if GzmB/SPB9 axis also affects the sensitivity of PCa as well as other cancer types to other chemotherapeutic drugs
POEM represents an effective nanocarrier in codelivery of GEM and siRNA (Fig. 3)
The pyrimidine structure is critical in stabilizing the siRNA NPs through π-π stacking and hydrogen bonding
It is possible that the hydroxyl groups in the sugar ring are also important in promoting the interaction with siRNA
albeit less important compared to pyrimidine motif
The use of two individual polymers (PPO and PPOGEM) each with cationic (-NH2) and GEM motif
will provide the flexibility of adjusting their ratio in formulation optimization
the very similar structure of the two polymers will facilitate their mixing to form compact and stable micelles
Although this study focuses on evaluating combination of GEM and siRNA
this strategy can be applied to codelivery of siRNA with other nucleoside analogue-based drugs such as AZA
other drugs such as cisplatin can be readily incorporated into POEM NPs following lipid-derivatization
our system may be tailor-designed to develop precision medicines to suit different combination therapies
may also play a role in enhancing the accumulation and penetration of POEM NPs
EPR shall also contribute to the tumor targeting by POEM NPs as well
especially considering their compact sizes (40–50 nm)
The combination of EPR-mediated passive targeting and fibronectin-mediated active targeting contributes significantly to the effective tumor accumulation of POEM NPs in both subcutaneous and orthotopic models: around 6% of injected siRNA formulated in POEM NPs was found in the tumor tissues at 24 h
and the siRNA concentrations in tumors were 3–4 folds higher than those in liver
More mechanistic studies on tumor targeting may lead to further improved tumor delivery systems in the future
More studies on the differential effect of different formulations and/or drug combinations on tumor cells and different immune cell subpopulations may lead to the development of an improved therapy targeting the GzmB/SPB9 axis
All animals were housed under pathogen free conditions according to AAALAC (Association for Assessment and Accreditation of Laboratory Animal Care) guidelines
All animal-related experiments were performed in full compliance with institutional guidelines and approved by the Animal Use and Care Administrative Advisory Committee at the University of Pittsburgh under protocol number 21099779
The maximum tumor volume permitted by the IACUC guidelines was 2000 mm3
tumor size and animal health were monitored daily
and the maximum allowed tumor burden was not exceeded
and KPC-C2-Luc cells were produced by following lentiviral/retroviral infection protocol as detailed in lentiviral infection section below
Panc02 and PANC-1 were cultured in DMEM supplemented with 10% fetal bovine serum (FBS) and penicillin/streptomycin (100 U/ml)
and KPC-C5 were cultured in DMEM supplemented with 10% fetal bovine serum (FBS)
1% GlutaMAX (100×) and penicillin/streptomycin (100 U/ml)
MIA PaCa-2 was cultured in DMEM supplemented with 10% fetal bovine serum (FBS)
Panc 02.03 and Panc 10.05 were cultured in RPMI-1640 supplemented with 15% fetal bovine serum (FBS)
Gemcitabine resistant cell lines were cultured in the full medium with gemcitabine (260 ng/mL)
All cells were cultured at 37 °C in a humidified atmosphere with 5% CO2
Female C57BL/6 mice aged between 4–6 and 8–10 weeks were purchased from The Jackson Laboratory (ME
Mice were housed at an ambient temperature of 22 °C (range: 22–24 °C) and a humidity of 45%
with a 14/10 day/night cycle (lights on at 6:00
Edit-R Mouse Serpinb9 mCMV-EGFP All-in-one Lentiviral sgRNA was purchased from Horizon Discovery Ltd
psPAX2 and pMD2.G were kindly provided by Dr
pLentipuro3/TO/V5-GW/EGFP-Firefly Luciferase Plasmid was purchased from Addgene (MA
SERPINB9 KO cell lines were generated by using CRISPR technology
Cells were infected with the lentivirus packaged by Serpinb9-All-in-one lentiviral sgRNA-CRISPR-Cas9 plasmid encoding EGFP
The successfully knocked out cells were selected by cell sorting of EGFP+ population
followed by single clone culture and further confirmed through Western blot analysis for the lack of SERPINB9 proteins
SERPINB9 control vector cell line was generated by using a control lentiviral vector with Cas9 coding sequence but without the specific guiding sequences (Lenti CRISPR plasmid without sgRNA sequence)
The luciferase-expressing cell lines were generated according to a published protocol56
Cells were infected with the lentivirus packaged from pLentipuro3/TO/V5-GW/EGFP-Firefly Luciferase plasmid encoding EGFP
The luciferase-expressing cells were selected by cell sorting of the EGFP+ population
and further confirmed through flow cytometry analysis for EGFP expression
To examine the mRNA level of different genes from RNA-seq results
murine pancreatic cancer cell lines (Panc02
and KPC-C5; WT vs GEMR) were collected and subjected to qRT-PCR as detailed below
To examine the effect of GEM on the mRNA level of GranzymeB
different pancreatic cancer cells were treated with various concentrations of GEM
Cells were collected 24 or 48 h later and subjected to qRT-PCR as detailed below
The total protein was extracted from the indicated cells by using radioimmunoprecipitation assay (RIPA) lysis buffer (Thermo Fisher Scientific
USA) through gently shaking on ice for 30 min
After centrifugation at 12,500 × g for 10 min
and the concentrations of proteins were determined using a Pierce BCA Protein Assay Kit (Thermo Fisher Scientific
The protein samples were mixed with 5× SDS loading buffer
loaded onto 10% SDS-polyacrylamide gel electrophoresis (PAGE) gel for electrophoresis
The membranes were then blocked in 3% BSA dissolved in phosphate buffer containing 0.05% Tween-20 (PBST) for 1 h at room temperature
the membranes were incubated with primary antibody in diluted buffer (3% BSA in PBST) with gentle agitation overnight at 4 °C
the membranes were subsequently incubated with horseradish peroxidase-conjugated secondary antibody at room temperature for 1 h
The membranes were then washed three times with PBST before being incubated with Pierce ECL Western Blotting Substrate (Thermo Fisher Scientific
Signal was visualized by films with the AX700LE film processor (Alphatek) or iBright™ FL1500 Imaging System
Granzyme B activity was measured using the GranToxiLux PLUS kit
Cells subjected to different treatments were incubated with the Granzyme B substrate for 1 h at 37 °C
The cleaved Granzyme B substrate (GranToxiLux) exhibited an excitation peak at 488 nm and an emission peak at 520 nm
GranToxiLux fluorescence was measured by flow cytometry
and cell populations positive for GranToxiLux were considered to have active Granzyme B
The three DNA fragments with different 5x repeated sequences were synthesized by AZENTA (MA
USA) and HindIII (Thermo Fisher Scientific
USA) restriction enzymes were used to digest the pGL3-Basic plasmid and the synthesized fragments
The 3 DNA fragments were individually ligated with the backbone by using T4 DNA ligase (Invitrogen
Single colonies were picked and expanded in the DH5α competent cells (Thermo Fisher Scientific
the concentration was determined by NanoDrop
and the sequence was confirmed by Sanger sequence
a full length promoter sequence containing all three binding motifs was synthesized by Twist Bioscience (CA
The mutated plasmid was constructed through site-directed mutagenesis
a pair of primers for mutagenesis were designed and synthesized (IDT
This pair of primers was designed to include the front and back sequence of each binding motif but without the motif sequence
Then the PCR reaction with this pair of primers was performed using the previously generated full-length plasmid as a template
The PCR product was treated with Dpn1 enzyme to remove the template
the PCR product was used for the transformation in DH5α competent cells
The Sanger sequencing confirmed the sequence
and Panc 02.03 cells were transfected with each of the plasmids described above using Lipofectamine 3000 (Invitrogen
the cells were treated with gemcitabine for an additional 48 h
Cell lysis was performed using the lysis buffer from the Pierce Firefly Luciferase Glow Assay Kit (Thermo Fisher Scientific
and bioluminescence was detected using a luminometer
according to the manufacturer’s instructions
Cytotoxicity was evaluated by MTT assay with indicated cell lines
Cells were seeded in 96-well plates (attached 96 well tissue culture plate (CELLTREAT
MA)) at a density of 2 × 103 cells/well with 100 μL of culture medium
Cells received various treatments including GEM alone
or GEM+siSPB9 combination at various GEM and siRNA concentrations for 48 h
cells were transfected with siRNA using Lipofectamine RNAiMAX (Invitrogen
USA) for 48 h followed by drug treatment for another 48 h
MTT assay was then performed on the cultured cancer cells
The absorbances of each well were measured at 590 nm
The cell viability was determined via the following formula: (ODtreated- ODblank)/(ODcontrol-ODblank) × 100 %
Cells were digested following different treatments for 24 h and stained with Zombie NIR and BV421 anti-mouse Annexin V or FITC anti-mouse Annexin V for flow cytometry analysis
Annexin V+ population was considered apoptotic cells
To synthesize PPO polymers conjugated with various amino acids
tert-butyloxycarbonyl (BOC)-protected amino acids (histidine
The activation of the amino acid carboxyl groups was achieved by adding 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide (EDC) and N-hydroxysuccinimide (NHS)
The reaction mixture was stirred for 2 h to promote conjugation
the non-amino acid-decorated PPO polymer and triethylamine (TEA) were introduced
and the mixture was stirred for an additional 12 h
The reaction product was purified by dialysis using a dialysis membrane (MWCO 3500 Da)
Dialysis was performed in a DMSO/H2O (4:1) mixture for 24 h
The final product was lyophilized and stored at 4 °C
The content of gemcitabine in the polymer was determined by UV absorbance
The conjugation rates of cytidine and glucosamine were determined by UV absorbance
To prepare the POEM/siRNA or Psugar/PPO/siRNA NPs
SiRNA was dissolved in deionized water at a concentration of 25 μg/mL
The DMSO solutions of PPO with PPOGEM or Psugar were prepared at different ratios
followed by rapid addition of siRNA (10 μg) aqueous solution
The mixture was centrifuged using an Amicon Ultra centrifugal filter device at 15,000 × g for 15 min
and the centrifugation was repeated at 15,000 g for 15 min to remove residual DMSO
The final nanoparticles in the remaining liquid in the tube were collected for subsequent studies
To assess the resistance of POEM/siRNA NPs against nuclease-mediated degradation
the NPs were incubated with RNase (50 U/mL) (NEB
and the integrity of siRNA was evaluated by electrophoresis
while the OL3 and OL15 force fields were used to model RNA and DNA
Initial system relaxation was achieved by a 1000-step conjugated-gradient energy minimization on the entire POEM/siRNA structure
constant-pressure MD simulation was performed for ~3.5 nanoseconds (ns)
facilitating system shrinking and stabilization
with an objective of achieving a density close to 1
a two-stage MD simulation protocol was applied to the shrunk system
with a 600 ns MD simulation to continue to stabilize the system in stage one
the last snapshot was solvated in a rectangular water box filled in with TIP3P water and 0.15 M Na+ and Cl− ions
The whole system was neutralized and the simulation box has a dimension of 220 × 220 × 220 Å
Then a 300 ns MD simulation was conducted with period boundary condition enforced in the second stage
position restraints were applied to the siRNA with a force constant of 100 kcal/mol/Å2 to prevent its distortion
but the other atoms were allowed to move freely
The snapshot with the smallest root-mean-square deviation (RMSD) from the average structure of snapshots collected after the system reached equilibrium (the last 150 ns) was selected as the representative conformation
A similar protocol was applied for the PCytidine/siRNA and Psugar/siRNA system
Samples were initially examined using negative-stain electron microscopy
A 3 μL aliquot was applied to a freshly glow-discharged continuous carbon copper grid and stained with 1% uranyl acetate solution
The grids were then inserted into a Tecnai TF20 electron microscope (Thermo Fisher Scientific
and images captured using an XF416 CMOS camera (TVIPS GmbH
Germany) to assess nanoparticle uniformity and concentration
3 μL of the sample was pipetted onto a Protochips C-flat CF-2/1-3CU-T grid (Protochips
USA) that had been glow discharged at 25 mA for 30 s using an Emitech KX100 glow discharger
The grids were then processed in a Thermo Fisher Vitrobot Mk 4
They were blotted for 3 s with a force setting of 4 and subsequently plunged into a 40/60 mixture of liquid ethane/propane that was precooled in a liquid nitrogen bath
The grids were then placed onto a Gatan 910 3-grid cryoholder (Gatan
USA) and inserted into the TF20 microscope
maintaining a temperature of no higher than −175 °C throughout
with contrast enhanced by a 100 μm objective aperture
Cryo-electron micrographs were collected at a nominal magnification of 150,000× on the TVIPS XF416 CMOS camera
Low dose methods were employed to minimize electron beam damage
and images were acquired using TVIPS EMplified software in movie mode to correct for drift
To test the in vitro knockdown efficiency of POEM NPs
KPC-C2-Luc and Panc02-Luc cells were treated with different formulations of POEM NPs with varying ratios of PPOGEM and PPO
cell lysates were collected and analyzed by measuring the bioluminescent intensity
Commercial Lipofectamine RNAiMAX was used as a control
KPC C2 WT cells were pretreated with chlorpromazine
The cells were then incubated with POEM/siRNA/DiD dye NPs for 1 h
and the fluorescence intensity of DiD dye was measured
KPC C2 cells were seeded into the upper chamber of a transwell and cultured for 3 days until a confluent monolayer was formed
Prior to adding POEM/siRNA/DiD NPs to the upper chamber
the cells were pretreated with anti-ITGA5 or IgG for 1 h
the medium in the lower chamber was collected
followed by measurement of its fluorescence intensity
To establish the subcutaneous tumor models
or KPC-C2 GEMR cells were inoculated into the right flank of C57BL/6 mice (4-6 weeks)
or KPC-C2 GEMR tumor-bearing mice received different treatments when the tumor size reached the indicated volume
Tumor growth in KPC-C2 SERPINB9 KO or KPC-C2 control vector tumor-bearing mice was monitored for 20 days
followed by analysis of tumor-infiltrating immune cells as detailed in “Analysis of tumor-infiltrating immune cells” section
anesthetized C57BL/6 mice (8–10 weeks) were shaved
and the surgical area on the left flank was disinfected
The pancreas was exposed through a small incision (~1 cm) on the left flank
Fifty microliters Panc02-Luc or KPC-C2-Luc single cell suspension (1 × 105 per mouse) was injected cell into the tail of the pancreas using 28-gauge hypodermic needles
The needle was slowly removed after the injection of cell suspension
the mice were maintained at the heating pad and observed until complete recovery
The development of pancreatic cancer was monitored by bioluminescence radiance intensity after the mice were injected with D-Luciferin (GoldBio
mice bearing subcutaneous (~300 mm3) or orthotopic (~10 days after inoculation) pancreatic tumors were intravenously injected with free siSPB9-cy5.5 and POEM/siSPB9-cy5.5 NPs with different PPOGEM/siRNA ratios
The mice were sacrificed at 24 h after injection
and kidney were collected and imaged by IVIS 200 system (Perkin Elmer
USA) at a constant 1 s exposure time with excitation at 679 nm and emission at 702 nm
blood was collected in EDTA-containing tubes at 10 min
48 h and 72 h timepoints and plasma samples were prepared by centrifugation at 21,000 × g for 10 min and imaged by the IVIS 200 system
Groups of 3 C57BL/6 mice (4–6 weeks) bearing subcutaneous KPC-C2 tumors (~300 mm3) received tail vein injection of POEM/siSPB9-cy5.5 NPs or free siSPB9-cy5.5 at a dose of 1 mg/kg for siRNA
blood was collected in the tubes containing EDTA
The amount of siRNA in the plasma was quantified by qRT-PCR as detailed below
The PK parameters were obtained by fitting the blood siRNA concentration versus time using a one-compartment model
and tumors were collected at 24 h and homogenized
SiRNA in the tissues was quantified through qRT-PCR
Spleen and KPC-C2 tumor tissues were harvested from C57BL/6 mice
followed by the preparation of single-cell suspensions
CD4+ and CD8+ T cells were isolated using CD4/CD8 MicroBeads (Miltenyi Biotec
Cells were cultured in RPMI-1640 medium and stimulated by anti-CD3 (Invitrogen
or Lipofectamine RNAiMAX/siSPB9-cy5.5 as a control for 4 h
Cellular uptake of siRNA was examined by flow cytometry
POEM NPs loaded with luciferase siRNA (siLuc) or control siRNA (siCT) were intravenously injected into KPC-C2-Luc tumor-bearing mice at a dose of 1 mg/kg
The efficiency of gene knockdown was measured three times by whole body bioluminescence imaging on the 2nd day following the 1st
and 3rd injection of the NPs once every 3 days
The exposure time was set at 60 s for every experiment
Mice were anesthetized according to protocol prior to imaging
KPC-C2 tumor-bearing mice were randomly assigned to different groups (n = 5)
They were intravenously administered with PBS
or POEM/siSPB9 NPs three times at an interval of 5 days (on day 5
The doses for PPOGEM and siRNA were 50 mg/kg and 1 mg/kg
Twenty-four hours after the final injection
tumors were collected and subjected to qRT-PCR of SPB9 expression as detailed above
Murine pancreatic cancer (KPC-C2 and KPC-C2 GEMR) models were established for in vivo antitumor efficacy study
every 3 days for a total of 5 times (PCytidine: 50 mg/kg; PPOGEM: 50 mg/kg; siSPB9: 1 mg/kg) through intravenous injection
Tumor volumes and mouse body weights were monitored every 3 days following the initiation of the treatment
The tumor volumes (V) were calculated by the formula: (Length × Width2)/2
tumor tissues and major organs were harvested for histochemical staining
and plasma was isolated after centrifugation at 21,000 × g for 10 min
and creatinine levels in plasma were measured as indicators of hepatic and renal function
the KPC-C2-Luc tumor-bearing mice were treated intravenously with PBS
The treatments were conducted every 3 days for a total of five times
The whole-body tumor burden was monitored and quantified by measuring the luminous intensity using Living Imaging 4.1.0 software
To test the therapeutic effect of the combinational therapy of POEM/siSPB9 NPs with anti-PD-1
the treatment was started when the KPC-C2 GEMR tumors reached ~50 mm3 in size
Mice were treated with anti-PD-1 (clone RMP1-14
while POEM/siSPB9 NPs were given intravenously at dosage described above
Mice were followed until death or were killed if the tumor size reached 2000 mm3
the maximal tumor size permitted by the Animal Use and Care Administrative Advisory Committee at the University of Pittsburgh
The images were observed under a BZ-X710 Fluorescence Microscope (Keyence
tumors were dissected and transferred into RPMI-1640 medium
Tumors were disrupted mechanically using scissors
digested with a mixture of deoxyribonuclease I (0.3 mg/mL
Sigma-Aldrich) and TL Liberase (0.25 mg/mL
Roche) in serum-free RPMI-1640 at 37 °C for 30 min
and dispersed through a 40 μm cell strainer (BD Biosciences)
live/dead cell discrimination was performed using a Zombie NIR Fixable Viability Kit (BioLegend
dilution: 1/1000) at 4 °C for 30 min in PBS
Surface staining was performed at 4 °C for 30 min in FACS staining buffer (1× PBS/5% FBS/0.5% sodium azide) containing designated antibody cocktails (PerCP anti-mouse CD45 antibody
Brilliant Violet 737 anti-mouse CD4 antibody
Brilliant Violet 480 anti-mouse CD8 antibody
Brilliant Violet 615 anti-mouse PD-1 antibody
Brilliant Violet 510 anti-mouse Gr-1 antibody
Brilliant Violet 737 anti-mouse CD80 antibody
FITC anti-mouse CD69; dilution: 1/200 for all antibodies)
Cells were fixed and permeabilized using the BD Cytofix/Cytoperm kit
For intracellular cytokine staining (PE-Cyanine7 anti-mouse IFN-γ antibody and eF450 anti-mouse GzmB antibody; dilution: 1/200 for antibody)
cells were stimulated with phorbol 12-myristate-13-acetate (100 ng/mL) and ionomycin (500 ng/mL) for 6 h in the presence of Monensin
Cells were fixed/permeabilized using the BD Cytofix/Cytoperm kit before cell staining
Statistical analysis was performed with two-tailed Student’s t-test for comparison between two groups
one-way analysis of variance (ANOVA) for comparison between multiple groups
and log-rank (Mantel–Cox) test for survival analysis as indicated in figure legend
Results were considered statistically significant if P < 0.05
Prism 10.1.0 (GraphPad Software) was used for data analysis and graph plotting
All experiments were repeated at least three times with similar results
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
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This work was supported by the fund from National Institute of Health grants R01CA219399
R01GM147673 (to J.W.) and The David and Betty Brenneman Scholar Fund (to S.L.)
This research used the Olympus FV3000 Confocal Microscope
which is supported by 1S10OD030254-01A1 (to RBG)
The Pittsburgh Center for CryoEM (RRID:SCR_025216) used for data collection in this project was supported
These authors contributed equally: Haozhe Huang
Department of Pharmaceutical Sciences and Computational Chemical Genomics Screening Center
The authors declare no competing interests
Nature Communications thanks Philippe Soubeyran
reviewer(s) for their contribution to the peer review of this work
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations
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AGO-clade Argonaute proteins utilize small interfering RNAs (siRNAs) as guides to recognize target with complete complementarity
resulting in target RNA cleavage that is a critical step for target silencing
These proteins feature a constricted nucleic acid-binding channel that limits base pairing between the guide and target beyond the seed region
How the AGO–siRNA complexes overcome this structural limitation and achieve efficient target cleavage remains unclear
We performed cryo-electron microscopy of human AGO–siRNA complexes bound to target RNAs of increasing lengths to examine the conformational changes associated with target recognition and cleavage
conformational transition propagates from the opening of the PAZ domain and extends through a repositioning of the PIWI–L1–N domain toward the binding channel
facilitating the capture of siRNA–target duplex
Subsequent extension of base pairing drives the downward movement of the PIWI–L1–N domain to enable catalytic activation
further base pairing toward the 3′ end of siRNA destabilizes the PAZ–N domain
which might facilitate the multi-turnover action of the AGO–siRNA enzyme complex
the “uni-lobed” structure of the AGO complex makes multiple contacts with the target in the central region of the siRNA–target duplex
Our findings shed light on the stepwise mechanisms by which the AGO–siRNA complex executes target RNA cleavage and offer insights into the distinct operational modalities of AGO and PIWI proteins in achieving such cleavage
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Argonaute proteins: Functional insights and emerging roles
Emerging roles and functional mechanisms of PIWI-interacting RNAs
Sorting of Drosophila small silencing RNAs partitions microRNA* strands into the RNA interference pathway
PIWI-interacting RNAs: small RNAs with big functions
indicates that thousands of human genes are microRNA targets
Origins and mechanisms of miRNAs and siRNAs
MRNA destabilization is the dominant effect of mammalian microRNAs by the time substantial repression ensues
Ribosome profiling shows that miR-430 reduces translation before causing mRNA decay in zebrafish
MicroRNA inhibition of translation initiation in vitro by targeting the cap-binding complex eIF4F
miRNA-mediated gene silencing by translational repression followed by mRNA deadenylation and decay
Kinetic analysis of the RNAi enzyme complex
RNAi in human cells: Basic structural and functional features of small interfering RNA
siRNA function in RNAi: A chemical modification analysis
RNAi: Double-stranded RNA directs the ATP-dependent cleavage of mRNA at 21 to 23 nucleotide intervals
RNA interference is an antiviral defence mechanism in Caenorhabditis elegans
RNA interference directs innate immunity against viruses in adult Drosophila
A dicer-independent miRNA biogenesis pathway that requires Ago catalysis
A novel miRNA processing pathway independent of dicer requires argonaute2 catalytic activity
Conserved vertebrate mir-451 provides a platform for Dicer-independent
Dual strategies for argonaute2-mediated biogenesis of erythroid miRNAs underlie conserved requirements for slicing in mammals
The structure of human argonaute-2 in complex with miR-20a
RISC is a 5′ phosphomonoester-producing RNA endonuclease
Argonaute divides its RNA guide into domains with distinct functions and RNA-binding properties
High-throughput analysis reveals rules for target RNA binding and cleavage by AGO2
a site-specific DNA-guided endoribonuclease
provides insights into RISC-mediated mRNA cleavage
Crystal structure of argonaute and its implications for RISC slicer activity
Crystal structure of a PIWI protein suggests mechanisms for siRNA recognition and slicer activity
propagation and cleavage of target RNAs in Ago silencing complexes
A biochemical framework for RNA silencing in plants
A microRNA in a multiple-turnover RNAi enzyme complex
Molecular basis for target RNA recognition and cleavage by human RISC
Structural insights into RNA cleavage by PIWI Argonaute
Water-mediated recognition of t1-adenosine anchors Argonaute2 to microRNA targets
Structure of an argonaute silencing complex with a seed-containing guide DNA and target RNA duplex
Structure-based cleavage mechanism of Thermus thermophilus argonaute DNA guide strand-mediated DNA target cleavage
RNAi: The nuts and bolts of the RISC machine
Purified Argonaute2 and an siRNA form recombinant human RISC
Highly complementary target RNAs promote release of guide RNAs from human argonaute2
A cellular function for the RNA-interference enzyme dicer in the maturation of the let-7 small temporal RNA
Control of stress-dependent cardiac growth and gene expression by a microRNA
Kinetic analysis reveals the fate of a microRNA following target regulation in mammalian cells
The structural basis for RNA slicing by human Argonaute2
Sarkar, S., Gebert, L. F. R. & MacRae, I. J. Structural basis for gene silencing by siRNAs in humans. bioRxiv https://doi.org/10.1101/2024.12.05.627081 (2024)
Structural basis for target-directed microRNA degradation
The guide-RNA sequence dictates the slicing kinetics and conformational dynamics of the Argonaute silencing complex
Crystal structure of silkworm PIWI-clade argonaute Siwi bound to piRNA
Mammalian PIWI–piRNA–target complexes reveal features for broad and efficient target silencing
GTSF1 accelerates target RNA cleavage by PIWI-clade Argonaute proteins
RNA clamping by Vasa assembles a piRNA amplifier complex on transposon transcripts
elegans VASA homologs control Argonaute pathway specificity and promote transgenerational silencing
Rapid and specific purification of Argonaute-small RNA complexes from crude cell lysates
CryoSPARC: Algorithms for rapid unsupervised cryo-EM structure determination
RELION: Implementation of a Bayesian approach to cryo-EM structure determination
Coot: Model-building tools for molecular graphics
PHENIX: A comprehensive Python-based system for macromolecular structure solution
UCSF Chimera — A visualization system for exploratory research and analysis
UCSF ChimeraX: Meeting modern challenges in visualization and analysis
Download references
Dangsheng Li for insightful suggestions; members of Shen’s lab for discussions; Cryo-EM Facility of Westlake University for providing support on cryo-EM data collection
This work was supported by Westlake Education Foundation
Zhejiang Provincial Foundation of China (2021R01013)
the National Natural Science Foundation of China (32070628)
Westlake Education Foundation (041010140118)
Zhejiang Provincial Key Laboratory Construction Project
and the Westlake Laboratory of Life Sciences to E.Z.S.
the National Natural Science Foundation of China (32271261)
Zhejiang Provincial Natural Science Foundation of China (LR22C050003)
and Institutional Startup Grant from the Westlake Education Foundation (101486021901) to J.W
These authors contributed equally: Zhenzhen Li
Key Laboratory of Growth Regulation and Translational Research of Zhejiang Province
Westlake Laboratory of Life Sciences and Biomedicine
Key Laboratory of Structural Biology of Zhejiang Province
Department of Pharmacology and Cancer Biology
performed experiments and analyzed the data
wrote the manuscript with help from all authors; H.G.
Overview of cryo-EM density and the structural model of hAGO2D669A-siRNA-target (12-nt)
Overview of cryo-EM density and the structural model of hAGO2D669A-siRNA-target (14-nt
Conformational dynamics of hAGO2 ternary complexes as complementarity extended towards the siRNA 3ʹ end
Conformational dynamics of MILI ternary complexes as complementarity extended towards the piRNA 3ʹ end
a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law
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DOI: https://doi.org/10.1038/s41422-025-01114-7
Multidrug-resistant bacteria pose a major threat to human health
Manipulation of bacterial genes at the transcriptional level is a potential strategy to fight antibiotic-resistant bacterial infections by silencing their resistance genes
siRNAs have not been applied to regulate bacterial genes due to the lack of RNAi regulatory machinery
efficient methods for delivering siRNAs to bacteria in vivo are not currently available
the authors demonstrated that exosomes can serve as delivery vehicles to introduce AGO2-loaded siRNA into the cytoplasm of bacteria
and in turn down-regulated gene expression of the mRNA that shares sequence complementarity to the siRNA
The scientific significance of these findings is highlighted below:
(1) Exosomal siRNA inhibits bacterial gene translation in an AGO2-dependent manner
Despite the fact that the siRNA machinery is absent in prokaryote
this study demonstrates that exosomal siRNAs can be efficiently delivered into bacteria and silence target bacterial genes
The exosomal Argonaute 2 (AGO2) protein forms a complex with siRNAs
which is essential for siRNA-mediated gene silencing in bacteria
Even though the delivered siRNA was designed for possessing full sequence complementarity to the bacterial mRNA
downregulation of the target protein was achieved at the translational level rather than on the level of mRNA stability (as would be expected in mammalian systems)
(2) Exosomal siRNA converts MRSA into methicillin-sensitive bacteria
Exosomal siMecA (an siRNA designed to target the mecA gene) can downregulate the mecA gene which encodes the penicillin-binding protein 2a (PBP2a)
a protein at the heart of the drug-resistance phenotype in MRSA
Both in vitro and in vivo (using MRSA-infected mice) data demonstrated that by reducing PBP2a levels by exosome-delivered siRNA-AGO2 complex
MRSA can be converted into methicillin-sensitive bacteria
(3) In vivo self-assembled siRNAs protect mice from lethal MRSA infection: potential clinical application
the authors demonstrated that by intravenous injection of a plasmid encoding all relevant genes for the production of a particular siRNA into mice
the mouse liver was producing siRNA-AGO2 loaded exosomes (siMecA-Exos) efficiently targeting MRSA
These findings have huge potential clinical relevance since it might be possible to use this approach to also target multi-drug resistant bacterial infections in the human system
(4) Exosome-mediated small RNA-AGO2 transport and bacterial gene silencing is a potential pathway by which mammalian cells regulate interacting bacteria in vivo
Nanjing University School of Life Sciences
Wang, C., et al. (2025). siRNA-AGO2 complex inhibits bacterial gene translation: A promising therapeutic strategy for superbug infection. Cell Reports Medicine. doi.org/10.1016/j.xcrm.2025.101997
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Lipid nanoparticles (LNPs) are widely used for nucleic acid delivery but face challenges like limited targeting and accelerated blood clearance (ABC) effect
We design three ionizable oligomers (IOs) that
with polylactide-polyethylene glycol (PLA-PEG)
The siRNA encapsulated IPMs escape from lysosomes upon cellular uptake
A fibroblast activation protein inhibitor modified IPMs (FAPi-IPMs) show higher targeting for activated hepatic stellate cells (HSCs) compared to that for hepatocytes
reducing collagen secretion and liver inflammation
IPMs and FAPi-IPMs mitigate ABC effect and produce fewer PEG antibodies than LNPs
and show minimal apolipoprotein adsorption in vivo compared with LNPs
differentiating their targeting effects from LNPs
IPMs represent a nucleic acid delivery system with alternative targeting ability and reduced ABC effect
current research is still confined within the scope of LNPs
unable to avoid the inherent problems of LNPs
current micelle-based nucleic acid delivery system has not made satisfactory progress
Three IOs with PEG-PLA were prepared by microfluidic chip to obtain IPM
siHSP47 and siHMGB1 were delivered to treat hepatic fibrosis by targeting activated hepatic stellate cells with the addition of FAPi-PEG-PLA in the formulation
attenuated ABC phenomenon of IPM was observed
a Schematic representation of different ionizable oligomers (IO) structures
c Particle size distribution of IPMs formed by different IOs with PEG5000-PLA8000
and encapsulation efficiency of IPMs at different N/P ratios (n = 3 samples)
IPM achieves the smallest particle size and PDI
along with higher encapsulation efficiency
and zeta potential of IPMs formed by different IOs (PEG5000-PLA8000) (n = 3 samples)
IPM (IOA2) exhibits the smallest particle size
and zeta potential of IPMs formed by different segment molecular weights of PEG-PLA (IOA2) (n = 3 samples)
IPM (PEG5000-PLA8000) shows the smallest particle size and highest encapsulation efficiency
g TEM images of IPMs formed by different IOs with PEG5K-PLA8K and nucleic acid stained by thionine
with IPM (IOA2) having the smallest particle size
and a higher concentration of RNA with a more punctate distribution
Values represent mean ± standard deviation (SD)
a Confocal microscopy images of HSCs co-incubated with IPM/Cy5-siNC formed by different IOs for 2 h
b Flow cytometry assay demonstrating the highest cellular uptake efficiency of IPM (IOA2
PEG5000-PLA8000) (n = 3 cell culture wells)
c The confocal images of the lysosomal escape experiments revealing a decline in the co-localization signals from 4 to 6 h
with LysoTracker Green labeling of lysosomes and Hochest 33342 labeling of nuclei
d Statistical analysis of Pearson’s R for co-localization of Cy5 signal with lysosomal signal
the Pearson’s R in the IPM (IOA2) group was <0.5
changing from moderate to low correlation (n = 3 cell culture wells)
e Statistical analysis of Overlap R for co-localization of Cy5 signal with lysosomal signal (n = 3 cell culture wells)
f TNS assay for the apparent pKa of the three blank carriers (n = 3 independent experiments)
g In vitro RNAi using IPM encapsulating siHSP47 and siHMGB1 formed by PEG5000-PLA8000 and IOA2
with LNP serving as a positive control and LNP/siNC serving as a negative control (n = 3 cell culture wells)
The qPCR results showing the effective silencing of the HSP47 (h) and HMGB1 (i) genes in vitro
with LNP and Lipo2000 serving as positive controls and LNP/siNC and no siRNA serving as negative controls (n = 3 cell culture wells)
Data were analyzed by One-way ANOVA followed by Tukey test
a GPC molecular weight distribution of FAPi-PEG5000-PLA8000 and PEG5000-PLA8000
b qPCR results demonstrating upregulation of FAP mRNA expression in HSCs following bleomycin stimulation (n = 3 cell culture wells)
c Flow cytometry analysis of the cellular uptake efficiency of IPM and FAPi-IPM by HSCs before and after bleomycin stimulation
being more effectively internalized by HSCs
with significant differences observed after bleomycin stimulation (n = 3 cell culture wells)
d Competitive inhibition assay with varying concentrations of free FAPi
showing dose-dependent cellular uptake of FAPi-IPM (n = 3 cell culture wells)
e Confocal microscopy results indicating increased intracellular fluorescence intensity in FAPi-IPM/Cy5-siNC-treated cells after bleomycin stimulation
with a decrease in intracellular fluorescence intensity as free FAPi concentration increases
f Western blot results of IPM/siHMGB1+siHSP47 and FAPi-IPM/siHMGB1+siHSP47 after bleomycin stimulation of HSCs
with LNP/siHMGB1+siHSP47 serving as a positive control
h Effective downregulation of target genes HSP47 and HMGB1 relative expression by IPM and FAPi-IPM (n = 3 cell culture wells)
i Schematic representation of hepatic fibrosis modeling
j ROI values in the liver of mice with hepatic fibrosis (n = 3 mice)
k Flow cytometry showing FAM positivity of activated hepatic stellate cells (α-SMA labeled) in the livers of mice with hepatic fibrosis (n = 3 mice)
l The immunofluorescence results of liver tissues from mice with hepatic fibrosis 24 h after the tail vein injection
with DAPI labeling of the nuclei and α-SMA labeling of activated hepatic stellate cells
m Fluorescence imaging of the liver 24 h after injection in mice with liver fibrosis
Data were analyzed by ANOVA followed by Tukey test
a Schematic representation of the dosing regimen for targeting hepatic stellate cells with FAPi-IPM co-delivery of siHSP47 and siHMGB1 for the treatment of hepatic fibrosis (n = 5 mice)
b H&E staining results of the liver showing histological changes
c Masson’s trichrome staining results of the liver demonstrating a reduction in collagen deposition area in the FAPi-IPM group
d Quantification of collagen deposition area
e Immunohistochemical staining for HSP47 in the liver showing a decrease in HSP47-positive area and expression in the FAPi-IPM group
g Immunohistochemical staining for HMGB1 in the liver showing a decrease in HMGB1-positive area and expression in the FAPi-IPM group
The FAPi group shows a decrease in ALT and AST levels to the normal range
with no significant difference compared with the negative control group
l Liver appearance showing changes in the PBS group and alleviation in the FAPi-IPM group
m Body weight curve of mice showing weight recovery after administration in the treatment groups
n Western blot results demonstrating inhibition of HSP47 and HMGB1 protein expression in the treatment groups
p Significant silencing of HSP47 and HMGB1 protein expression in the FAPi-IPM group in vivo
r qPCR results demonstrating significant gene silencing of HSP47 and HMGB1 in the treatment groups
Data were analyzed by ANOVA followed by Tukey’s multiple comparisons test
a Fluorescence imaging of healthy male C57BL/6 mice (6–8 weeks old) injected with FAPi-IPM
LNP enters the liver more rapidly and is rapidly cleared
while FAPi-IPM exhibits prolonged liver distribution
b Immunofluorescence staining of liver tissue (F4/80 labeling KCs) at 24 h post-injection reveals differences in uptake among formulations
c ROI values indicate LNP accumulates most in the liver at 4 h
whereas FAPi-IPM shows delayed liver accumulation at 24 h (n = 3 mice)
d Pearson’s R of FAM fluorescence and KCs in liver showing rapid phagocytosis of LNP by KCs at 2–4 h (n = 3 mice)
e Cell distribution changes show LNP is captured by hepatocytes and Kupffer cells at 2 h
while FAPi-IPM enters hepatocytes later at 8 h; IPM enters hepatocytes less overall (n = 3 mice)
all formulations are mainly taken up by mononuclear cells
with FAPi-IPM showing the highest uptake (n = 3 mice)
g The 2-h FAM colocalization results in the spleen indicate that all three formulations strongly colocalize with neutrophils and are mostly taken up by neutrophils
h Schematic representation of dosing regimen: PEGylated drug injections on days 0
with pharmacokinetic assays on days 1 and 10
and anti-PEG IgM levels assessed on days 1
i Pharmacokinetic curves of the three PEGylated drugs and pharmacokinetic curves rechallenged on day 10
AUC0-24 of the three PEGylated drug on day 1 (j) and day 10 (k)
l Ratio of AUC0-24 rechallenged and AUC0-24
a Schematic illustration of the process for isolating the in vitro and in vivo protein coronae adsorbed on formulations
b Silver staining results of protein coronae adsorbed on FAPi-IPM (F)
Three times was repeated independently with similar results
c–e Protein concentrations collected from the three PEGylated drugs via affinity chromatography columns
f The two tubes with the highest protein concentrations collected from each formulation via affinity chromatography columns were defined as the protein coronae adsorbed on the formulations
with FAPi-IPM and IPM exhibiting higher protein corona concentrations than LNP
g The number of protein types adsorbed on the three formulations
h Top 50 proteins adsorbed on the three formulations classified by complement
j Top 20 proteins adsorbed on the three formulations
Molecular function (k) and KEGG analyses (l) of the protein coronae adsorbed on IPM
Data were analyzed using one-way ANOVA followed by Tukey’s multiple comparison test
we successfully designed and synthesized three IOs formulations with potential for nucleic acid delivery
Through screening based on physicochemical properties
we optimized the formulation and developed a potential nucleic acid delivery system
we found that IOA2 with oligoalanine tails outperformed IOLA4 and IOLA8 with oligolactic acid tails
to the greater stability of amide bonds compared to ester bonds in vivo
along with the introduction of more nitrogen
it may be due to the shorter alkyl chain between the tertiary amine head group and the hydroxyl group
resulting in stronger protonation ability and enhanced capabilities for electrostatic adsorption of siRNA and escape from lysosomes
To apply this potential delivery system to the treatment of hepatic fibrosis using siRNA therapy targeting activated HSCs overexpressing FAP
we further introduced the targeting molecule FAPi
FAPi-IPM exhibited approximately 20% higher uptake by activated hepatic stellate cells compared with IPM
the RNAi efficiency targeting HSP47 and HMGB1 respectively increased to 55.39 ± 1.22% and 42.46 ± 3.49% respectively
FAPi-IPM showed significant targeting to hepatic stellate cells in mice with hepatic fibrosis
with reduced phagocytosis by KCs compared with IPM
leading to more effective knockdown of HMGB1 and HSP47
thus effectively alleviating hepatic fibrosis
we found that IPM achieved similar therapeutic effects compared with the positive control
To explore the differences in the in vivo fate of IPM compared with traditional LNP
we further investigated the biodistribution and pharmacokinetic performance of the three formulations
The results of biodistribution showed that
FAPi-IPM did not exhibit significant targeting ability
which may be related to the non-activation of HSCs and low expression of FAP in healthy mice
FAPi-IPM was less prone to phagocytosis by KCs and entered HSCs later than IPM
IPM and FAPi-IPM were more likely to be taken up by neutrophils than LNP
whereas LNP was more likely to be taken up by monocytes and DCs
This cellular distribution pattern may lead to faster clearance of LNP compared with IPM and FAPi-IPM
Pharmacokinetic results confirmed our hypothesis
FAPi-IPM and IPM were metabolized more slowly in the liver than LNP
with smaller serum clearance rate constants and longer half-lives
the titer of anti-PEG IgM produced by FAPi-IPM was much lower than that of IPM and LNP
IPM and LNP exhibited significant ABC effects
To further analyze the reasons for the different in vivo fates
we examined the differences in the composition and relative abundance of soft protein coronas adsorbed by the three formulations in vitro and in vivo
The results showed that FAPi-IPM and IPM adsorbed higher concentrations and more types of proteins in vitro and in vivo than LNP
The top 50 proteins adsorbed by FAPi-IPM and IPM contained fewer complement proteins and almost no apolipoproteins
and most of the adsorbed proteins were functionally related to binding
This explains why they are cleared more slowly in the serum
possibly due to rapid adsorption of proteins in the circulation
camouflaging themselves as non-“foreign” particles
thereby avoiding capture and clearance by the mononuclear phagocyte system
The composition of the top 50 proteins adsorbed by LNP differed significantly from the other two formulations
containing apolipoprotein E and complement component 3
and the function of the adsorbed proteins was related to oxidoreductase activity
with significant involvement in the complement pathway
revealing the rapid distribution in hepatocytes and rapid metabolism in vivo
ionizable oligomer structure modification is also significant for improving the capability of IPM
All animal experiments were conducted following guidelines approved by the Ethics Committee of East China Normal University (ARXM2023088)
SPF grade Male C57BL/6 mice aged 6–8 weeks were purchased from the Shanghai Laboratory Animal Center
The animals are kept in the Experimental Animal Center of the Institute of Brain Functional Genomics (license number: SYXK (Shanghai) 2014-0006)
and IVC independent air supply cages are used inside the barrier environment
Anesthetize mice with isoflurane: Adjust the induction concentration to 3–4%
wait for the anesthetic to fill the induction box
then close the induction box and wait for the animal to be completely anesthetized (this process takes about 2–3 min)
The induction box can be gently shaken to check if the animal is completely anesthetized
If the animal is flipped over to the side and has not attempted to return to its lying position
it indicates that the animal is completely anesthetized
mice were anesthetized with 10% chloral hydrate (0.004 ml/g body weight) intraperitoneally and euthanized for cervical dislocation to minimize animal pain
and the bodies are disinfected and placed in body bags
frozen and stored for harmless incineration as soon as possible
PEG-PLA and IOs were dissolved in anhydrous ethanol at a ratio of 40.2:59.8 (mol/mol) as the organic phase
while siRNA (N/P = 5.45) was dissolved in pH 5.0 10 mM citrate buffer as the aqueous phase
with twice the volume of the aqueous phase in pH 6.0 10 mM citrate buffer as the buffer phase
The aqueous phase and organic phase were mixed at a flow rate of 3:1 using a microfluidic device (NEXSTAR NANO2
The mixture was then centrifuged in ultrafiltration centrifuge tubes (MWCO = 10 kDa) at 2000 × g for 20 min three times
followed by elution with PBS and collection of the final product IPM
FAPi-IPM had a composition of PEG-PLA: ionizable oligomers: FAPi-PEG-PLA = 40.2:59.8:1 (mol/mol)
with the rest of the process remaining consistent
ALC-0315/DSPC/Chol/PEG2000-DSPE was dissolved in ethanol at a ratio of 50:10:38.5:1.5 (mol/mol) as the organic phase
siRNA (N/P = 5.67) was dissolved in pH 5.0 10 mM citrate buffer as the aqueous phase
and two times the volume of the aqueous phase in pH 6.0 10 mM citrate buffer as the buffer phase
C5-3 chips were selected and prepared by microfluidic instrumentation with an aqueous phase: organic phase at a flow rate of 3:1
centrifuged three times at 2000 × g for 20 minutes in ultrafiltration centrifuge tubes (MWCO = 10 kDa)
eluted by the addition of PBS and the collection of final products
Encapsulation efficiency was determined using Quant-iT Ribogreen RNA assay
Dynamic light scattering (DLS) technique was employed with Zetasizer Nano ZS (Malvern
UK) to measure the nanoparticle hydrodynamic radius
Transmission electron microscopy (TEM) JEOL 100-CX (JEOL USA Inc.
MA) was used to observe the morphology of nanoparticles
followed by staining of RNA with thionine (0.1 mM) to observe the inner position of nucleic acid drugs
Samples were prepared at a concentration of 0.5 mg/mL
The prepared formulation was co-incubated with 10% (v/v) serum
and the stability in serum was assessed by measuring the particle size within 7 days
The pKa of the micelles was determined using the TNS method
Blank nanoparticles were prepared and diluted in a series of citrate buffer solutions with pH ranging from 3 to 10 at a concentration of 6 μM
TNS was dissolved in DMSO at a concentration of 300 μM
and 2 μL of the TNS solution was mixed with 100 μL of blank nanoparticles
Fluorescence intensity was measured under excitation at 325 nm and emission at 435 nm
The fluorescence intensity readings were curve-fitted against the pH values to calculate the pKa
IPMs and LNP were co-incubated with HSCs for 2
The cells were stained with Hoechst 33342 for nucleus labeling and LysoTracker Green DND-26 for lysosome labeling
The changes in co-localization signals between Cy5 fluorescence and lysosomes were observed under a laser scanning confocal microscope (LEICA
Pearson’s R and Overlap R were calculated and analyzed
After co-incubation of micelle-encapsulated Cy5-siNC with activated HSCs for 6 h
flow cytometry was performed to measure Cy5+ cells and calculate the cellular uptake rate
stained with Hoechst 33342 for nucleus labeling
and sealed with anti-fluorescence quenching mounting medium
The Cy5 fluorescence signal in the cells was observed under a confocal microscope
HSCs activation was induced by culturing cells in medium supplemented with bleomycin (1 µg/mL) for 24 h
The medium was then replaced with opti-MEM
and IPM/siHSP47+siHMGB1 with or without FAPi targeting moiety was added for a 6-hour co-incubation
while protein was harvested after 72 h for Western blot analysis to assess RNAi efficiency at both the gene and protein levels
Male C57BL/6 mice aged 6–8 weeks were intraperitoneally injected with a 20% CCl4 solution in mineral oil (2 mL/kg body weight) three times per week for 12 consecutive weeks
Liver sections were evaluated for fibrosis scoring using the Metavir fibrosis scoring system
and the modeling was considered successful when the pathology of the mouse liver reached stage S3
Groups of control and hepatic fibrosis model mice (n = 3) were intravenously injected with FAPi-IPM and IPM which encapsulated Cy5-siNC (1 mg/kg)
and kidneys were harvested to observe the fluorescence signal intensity
Groups of control and hepatic fibrosis model mice (n = 3) were intravenously injected with LNP
FAPi-IPM or IPM which all encapsulated FAM-siNC (1 mg/kg)
Liver tissues were further processed for histological analysis
with α-SMA marking hepatic stellate cells (HSCs)
CD146 marking hepatic sinusoidal endothelial cells
The spleen was also examined for CD45-positive leukocytes and CD68-positive macrophages
The targeting for HSCs in the liver was evaluated
liver perfusion was performed to separate non-parenchymal cells
Activated HSCs were labeled with α-SMA recombinant mouse mAb
followed by staining with goat anti-mouse AF647 secondary antibody
The uptake rate of activated hepatic stellate cells in fibrosis liver was defined as the proportion of FAM-positive cells
C57BL/6 male mice with successfully established models were divided into four groups (n = 5): IPM/siHSP47+siHMGB1 with and without FAPi targeting moiety
Treatment was administered twice a week for two consecutive weeks (1 mg/kg)
serum levels of alanine transaminase (ALT)
and tumor necrosis factor-α (TNF-α) were measured and compared with pre-treatment levels
Liver and other major organs were harvested for H&E and Masson’s trichrome staining to observe collagen fiber proliferation
and qPCR (Bio Rad) were employed to detect the expression levels of HMGB1 and HSP47 proteins and genes in liver tissues
Male C57BL/6 mice aged 6–8 weeks were intravenously injected with LNP
and kidney were harvested for fluorescence imaging using a small animal live imaging system (Bruker Corporation)
Immunofluorescence staining was performed for liver and spleen tissues
α-SMA was used to label hepatic stellate cells (HSCs)
CD146 for liver sinusoidal endothelial cells
Co-localization analysis with FAM was conducted for each marker
FAPi-IPM or IPM which all encapsulated FAM-siNC RNA (1 mg/kg)
Liver tissue was minced and incubated at 37 °C for 0.5 h
then ground through a 70 μm cell strainer into a 50 mL centrifuge tube
The sample was washed with 15 mL ice-cold HBSS-CaCl2 and centrifuged at 4 °C
The supernatant was transferred to a new 50 mL tube for non-parenchymal cell isolation
while the pellet was washed twice with 15 mL ice-cold HBSS-CaCl2
The final pellet was resuspended in 1 mL PBS to obtain parenchymal cells
The supernatant for non-parenchymal cell isolation was further centrifuged at 4 °C
The cell pellet was resuspended in 1 mL PBS and gently layered on a 25% (2.5 mL)/50% (2 mL) Percoll gradient
The sample was centrifuged horizontally at 4 °C
The intermediate cell layer (2 mL) was collected
The pellet containing non-parenchymal cells was retained
Hepatocytes were labeled with albumin antibody
followed by staining with goat anti-rabbit BV421 secondary antibody
Liver sinusoidal endothelial cells were labeled with APC-CD146
the spleen was transferred to an EP tube with 1000 μL PBS
and ground through a 70 μm cell strainer into a six-well plate
and the cell suspension was collected and centrifuged at 4 °C
and 1 mL red blood cell lysis buffer was added to the cell pellet
The lysis step was repeated until all red blood cells were removed
cells were washed with ice-cold PBS and centrifuged at 4 °C
Spleen tissues were ground over a 70 μm cell strainer
and cell suspensions were collected and lysed
Dendritic cells were labeled by BV421-CD11c
NJ) was used to analyze the percentage of FAM+ cells
Enzyme-linked immunosorbent assay (ELISA) was performed to measure the titers of anti-PEG IgM antibodies
A high-binding 96-well plate was coated with mPEG 2000-DSPE at a concentration of 20 µg/mL in ethanol
The plate was then blocked with 5% BSA for 1 h
were added to the plate in a serial dilution manner
the plate was incubated with Goat Anti-Rat IgM mu chain (HRP) secondary antibody (ab97180) diluted 1:5000 in 0.1% BSA for 1 h at 37 °C
and the plate was incubated for 8 min for color development
The reaction was terminated with 0.18 M sulfuric acid
The optical density (OD) at 450 nm was measured using a microplate reader (Biotek)
The emulsion should be disrupted using methanol
after which the fluorescence intensity of FAM in the serum should be measured
A standard curve should be constructed based on the fluorescence intensity of the FAM-siNC
from which the concentration of siRNA can then be calculated
Using a previously reported method by Zhan’s lab50
20 µL of FAM-siNC-loaded micelles and LNP (maintained at the same concentration by fluorescence quantification) were separately mixed with 60 µL of His-tagged PEG-scFv (corresponding to 400 µg of antibody for micelles and 100 µg for LNP) and incubated at room temperature for 10 min
the mixtures were combined with 20 µL of C57BL/6 mouse serum and incubated in vitro at 37 °C for 30 min
FAPi-IPM or IPM which all encapsulated Cy5-siNC (1 mg/kg) (maintained at the same concentration by fluorescence quantification)
Blood samples (20 µL) were collected from the tail vein using EDTA anticoagulant
The samples were directly mixed with 60 µL of His-tagged PEG-scFv (same as before)
Ni-NTA was packed into a 3 mL gravity column
and the pre-mixed solutions were slowly applied to enable a complete interaction of Ni and His-tagged PEG-scFv for 30 minut at room temperature
Fractions #1-#12 were collected using PBS containing 5 mM imidazole (to wash out unbound protein components)
while fraction #13 onwards was eluted using 100 µL of PEG8000 in PBS (100 mg/mL) and collected into #14 for fluorescence fraction
The components collected from the three formulations were quantified using BCA assay
and two tubes were combined and denatured by adding 1/4 of 5× loading buffer and heating at 100 °C for 10 min
following SDS-PAGE separation with silver staining
Approximately 200 ng of total peptides from each sample were separated using a nanoUPLC liquid chromatography system (nanoElute2) coupled to a mass spectrometer equipped with a nanospray ion source (timsTOF Pro2)
Chromatographic separation was achieved using a 75 μm ID × 15 cm reversed-phase column (IonOpticks C18-CSI
The raw data files were searched against a database using the SpectroMine (4.2.230428.52329
Biognosys AG) software application Pulsar retrieval engine for qualitative analysis
label-free quantification was performed by summing the intensities of all peptides in the sample
The top 50 proteins in protein corona on the three nanocarriers were functionally categorized using the DAVID database
followed by Gene Ontology (GO) and Encyclopedia of Genes and Genomes (KEGG) analyses
Flow cytometry data were processed using FlowJo software
Laser confocal microscopy and immunofluorescence results were analyzed for colocalization using the Colocalization Finder plugin in ImageJ
Immunohistochemistry results were analyzed for positivity rates using the IHC plugin in ImageJ
The Split Channels function in ImageJ was used to convert images to single-color channel 8-bit grayscale images
and the average grayscale values were calculated to determine the average immunofluorescence intensity
The Color Threshold function in ImageJ was used to set ranges and calculate the collagen deposition area in Masson’s staining
All data are presented as mean ± standard deviation
Student’s t test (two-sided) was used to analyze data between two groups
analysis of variance (ANOVA) was conducted followed by Tukey’s multiple comparison test
Statistical significance was defined as ns (p > 0.05)
All data analyses were performed using GraphPad Prism v9.5 software
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
Liquid crystalline inverted lipid phases encapsulating siRNA enhance lipid nanoparticle mediated transfection
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Neurotransmitter-derived lipidoids (NT-lipidoids) for enhanced brain delivery through intravenous injection
Rational design of bisphosphonate lipid-like materials for mRNA delivery to the bone microenvironment
Lian, X. et al. Bone-marrow-homing lipid nanoparticles for genome editing in diseased and malignant haematopoietic stem cells. Nat. Nanotechnol. https://doi.org/10.1038/s41565-024-01680-8 (2024)
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polymeric micelle formulation of paclitaxel
with cisplatin in patients with advanced non-small-cell lung cancer
The histidine-rich peptide LAH4-L1 strongly promotes PAMAM-mediated transfection at low nitrogen to phosphorus ratios in the presence of serum
Polyethylenimine (PEI) in gene therapy: current status and clinical applications
Nanoparticle-delivered siRNA targeting Bruton’s tyrosine kinase for rheumatoid arthritis therapy
Dually regulating the proliferation and the immune microenvironment of melanoma: Via nanoparticle-delivered siRNA targeting onco-immunologic CD155
Drug delivery systems for RNA therapeutics
Updated key points of Guidelines for the diagnosis and management of hepatic encephalopathy in cirrhosis (2018)
The immunological and metabolic landscape in primary and metastatic liver cancer
Fibroblast growth factor 18 stimulates the proliferation of hepatic stellate cells
Practical diagnosis of cirrhosis in non-alcoholic fatty liver disease using currently available non-invasive fibrosis tests
Activated hepatic stellate cell-derived Bmp-1 induces liver fibrosis via mediating hepatocyte epithelial-mesenchymal transition
The m6A reader IGF2BP2 regulates glycolytic metabolism and mediates histone lactylation to enhance hepatic stellate cell activation and liver fibrosis
Identification of pyroptosis-related gene signature in nonalcoholic steatohepatitis
Inflammatory modulation of HSCs: viewing the HSC as a foundation for the immune response
Programmed cell death in hepatic fibrosis: current and perspectives
The intersection between alcohol-related liver disease and nonalcoholic fatty liver disease
HMGB1-induced autophagy facilitates hepatic stellate cells activation: a new pathway in liver fibrosis
Targeting hepatic macrophages to treat liver diseases
Osteopontin and HMGB1: novel regulators of HSC activation
Resolution of liver cirrhosis using vitamin A-coupled liposomes to deliver siRNA against a collagen-specific chaperone
Ligand-tethered lipid nanoparticles for targeted RNA delivery to treat liver fibrosis
Hepatic macrophage targeted siRNA lipid nanoparticles treat non-alcoholic steatohepatitis
Liver-Targeted siRNA lipid nanoparticles treat hepatic cirrhosis by dual antifibrotic and anti-inflammatory activities
Nanomaterial Delivery Systems for mRNA Vaccines
Rational design of cationic lipids for siRNA delivery
Branched-tail lipid nanoparticles potently deliver mRNA in vivo due to enhanced ionization at endosomal pH
Deciphering protein corona by scFv-based affinity chromatography
RNA interference by single- and double-stranded siRNA with a DNA extension containing a 3′ nuclease-resistant mini-hairpin structure
Shielding of lipid nanoparticles for siRNA delivery: Impact on physicochemical properties
Synergistic lipid compositions for albumin receptor mediated delivery of mRNA to the liver
Different kinetics for the hepatic uptake of lipid nanoparticles between the apolipoprotein E/low density lipoprotein receptor and the N-acetyl-D-galactosamine/asialoglycoprotein receptor pathway
Anionic lipid nanoparticles preferentially deliver mRNA to the hepatic reticuloendothelial system
Immunogenicity of lipid nanoparticles and its impact on the efficacy of mRNA vaccines and therapeutics
Bacteria-derived outer-membrane vesicles hitchhike neutrophils to enhance ischemic stroke therapy
Neutrophil hitchhiking for drug delivery to the bone marrow
Chemotaxis-driven delivery of nano-pathogenoids for complete eradication of tumors post-phototherapy
Long-range corrected hybrid density functionals with damped atom-atom dispersion corrections
Accurate pKa calculations for carboxylic acids using Complete Basis Set and Gaussian-n models combined with CPCM continuum solvation methods
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This work was supported by the National Natural Science Foundation of China (82373813 [Yan]
the National Key R&D Program of China (Grant No
Shanghai Frontiers Science Center of Molecule Intelligent Syntheses
These authors contributed equally: Ziyu Zhou
Institute of Biomedical Engineering and Technology
Shanghai Engineering Research Center of Molecular Therapeutics and New Drug Development
School of Chemistry and Molecular Engineering
Ministry of Education & Department of Pharmacy
Department of Pharmacology School of Basic Medical Sciences & State Key Laboratory of Molecular Engineering of Polymers
Eye Institute and Department of Ophthalmology
and Z.Y.: Conceived and designed the experiments
Nature Communications thanks the anonymous reviewers for their contribution to the peer review of this work
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DOI: https://doi.org/10.1038/s41467-024-55721-w
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The use of combinatorial siRNAs shows great promise for drug discovery
but the identification of safe and effective siRNA combinations remains challenging
we develop a massively multiplexed technology for systematic screening of siRNA-based cocktail therapeutics
We employ composite micro-carriers that are responsive to near infrared light and magnetic field to achieve photoporation-facilitated siRNA transfection to individual cells
randomized gene silencing by different siRNA formulations can be performed with high-throughput single-cell-based analyses
we test more than 1300 siRNA combinations for knocking down multiple genes related to tumor growth
discovering effective 3-siRNA formulations with an emphasis on the critical role of inhibiting Cyclin D1 and survivin
along with their complementary targets for synergic efficacy
This approach enables orders of magnitude reduction in time and cost associated with largescale siRNA screening
and resolves key insights to siRNA pharmacology that are not permissive to existing methods
which may diminish the action of a single siRNA and substantially offset the silencing effects
the selection of combinatorial siRNAs to form the most effective cocktail primarily relies on examining the silencing efficacy and safety of individual siRNAs
which is time-consuming and lacks the information regarding the synergic or counteractive function among them
it is challenging to screen different siRNA combinations and to determine the optimal cocktails
and systematic high-throughput platform technology would be greatly beneficial to enhance the clinical adoption and speed up the development of siRNA-based therapeutics
This work aims to address the unmet needs by developing a high-throughput technology for screening siRNA-based cocktail therapeutics in a massively multiplexed
we employ a multilayer functionalization of hierarchically assembled nano-/micro composite carriers (Knock-beads)
rendering them with responsiveness to near infrared light and magnetic field to facilitate photoporation-induced cellular transfection of RNAs with single cell encoding capability
randomized gene silencing by different siRNA variants is performed
Our technology is capable of scaling to screening hundreds or even thousands of siRNA cocktail formulations in a single well
accelerating the testing of siRNA cocktails
Such benefits are not just limited to reducing the time and cost associated with siRNA screening by powers of magnitude
but also answer fundamental siRNA questions that are not addressable by existing methods
we first perform a small screen with six cell apoptosis or cell cycle related siRNAs to test 54 siRNA combinations to seek the most effective cocktail for inhibiting cancer cell growth
With a customized multiplexed encoding strategy
we further demonstrate an expanded screening involving 20 siRNA target genes and test more than 1300 cocktail formulations composed of 1
or 3 siRNAs for combinatorial knockdown of genes related to tumor growth
leading to the identification of the most effective 3-siRNA combinations as potential anti-cancer therapeutics with an emphasis on the critical role of inhibiting Cyclin D1 and survivin
as well as their complementary gene targets for synergic co-operation
We believe that this study demonstrates the path to a systematic and high-throughput platform technology that is greatly useful to accelerate further development of siRNA-based therapeutics and enhance their clinical adoption
Fe3O4 beads are combined with Au nanorods and coated with PDDA
The Au layer provides Knock-beads with photothermal responsiveness
facilitating intracellular delivery of siRNA through photoporation by 980 nm NIR laser
Knock-beads are immobilized on top of cells
enabling efficient cellular transfection of siRNAs by photoporation and single-cell encoded gene silencing in a large number of cells
Through only one-shot assay in a cell culture
more than 1300 siRNA combinations can be simultaneously analyzed to reveal the optimal siRNA therapeutic cocktail
a multiscale assembly of micro- and nano- structures along with a functionalization scheme was developed to fabricate the Knock-bead with multiple functions
including magnetic controllability for tight cell-bead interfacing
appropriate surface coating for siRNA loading/off-loading
and responsiveness to near infrared light (NIR) for photoporation
performs 3 functions: (1) a vehicle for siRNA delivery; (2) a spatially resolvable cellular interface for immobilization on the cell membrane by a magnetic field; (3) the means for fluorescence encoding of single-cell gene silencing by different siRNA combinations
the total number of possible gene silencing combinations would be:
a The chemical synthesis route of Knock-beads
b SEM images showing the core part of Knock-beads at different scales: Fe3O4-Au (top
c Fluorescence image showing Fe3O4 magnetic beads that were first labeled with Alexa-647 dye and then conjugated to Au nanorods
d Fluorescence image showing the Au nanorods that were first labeled with Alexa-647 dye and then conjugated to Fe3O4 magnetic beads
e Dynamic light scattering results showing the size variation of Fe3O4
Fe3O4-Au-PDDA beads and Fe3O4-Au-PDDA-siRNA conjugates (8 × 105 beads
Fe3O4-Au-PDDA beads and Fe3O4-Au-PDDA-siRNA conjugates (8 × 105 beads
g Fluorescent image of Knock-beads in PBS solution
Three independent experiments were conducted (b
Source data are provided as a Source Data file
a UV absorbance spectrum of Au nanorods
b Infrared imaging of the photothermal effect of Knock-beads (top) and DI water (control
A 980 nm laser (16 μs pulse width) with an intensity of 0.6 W/cm2 was applied for 30 s
c Time—temperature graph of Knock-beads (red) or DI water (blue) when stimulated by 980 nm laser
d Impact of different NIR-irradiation times (2 s
and 12 s) on cell viability 24 h after photoporation with Knock-beads
e Characterization of siRNA loading efficiency of Knock-beads using prelabeled siRNAs pull-down assay
f The fluorescence distribution of a siRNA-loaded Knock-bead along the yellow line in panel (g)
g 3D fluorescence images of Knock-beads (blue) loaded with siRNA (red) and the top
For effective gene silencing screening, cell viability is crucial for unbiased results, especially after the photoporation using the Knock-beads. 24 h following NIR irradiation, we assessed cell viability using the 3-(4,5-dimethylthiazol-2-yl)−2,5-diphenyltetrazolium bromide (MTT) assay (Fig. 3d)
0.6 W/cm2) with varying irradiation times (2
the cell viability was evaluated to optimize the irradiation parameters
We found that more than 85% of the cells were viable after an 8 s NIR irradiation at 0.6 W/cm2; longer NIR irradiation of 10 s and 12 s reduced the cell viability to 70% and 55%
NIR irradiation duration was kept brief ( < 8 s) to avoid any major damage or interference to regular cell function
thus ensuring the reliability for later use for high-throughput screening
a–c Intracellular delivery with a magnetic field
where RNAs are labeled using cy5 (red) and Fam (green)
d Cell segmentation visualized by a customize algorithm
The cell outline was visualized in different colors to help cell segmentation
e Number of cells categorized differently in (d): control refers cells without Knock-beads
f 3D images of Knock-beads(green) and diffused siRNA(red) and the front and top view
g 3D images of Knock-beads(green) and cell actin(red) and the front and top view
h Cells treated with two types of Knock-beads: anti-actin (KB-A
i Magnified view of (h) cells that contacts with different Knock-beads: top-left is control
j Quantification of fluorescence intensity for actin and tubulin: control refers cells without Knock-beads
three independent experiments were conducted
These results establish the Knock-beads as a legitimate tool for high-throughput gene silencing with single-cell addressability
and strongly support the development of more complex assays to enable screening of combinatorial siRNA cocktails
a Effect of siRNA number on the induction of cellular apoptosis
b Effect of siRNA numbers on the inhibition of cellular proliferation
c Scattered plot showing the distribution of the knock-combo efficacy classified by the number of siRNAs
The dotted line (f(x) = x) refers to the total anti-tumor efficacy with equal weight of cellular apoptosis and proliferation in determining the final efficacy
Comparison between single or dual pathway gene silencing by different Knock-combos composed of 3 (d) or 2 (e) siRNAs
The black dots indicate the measurements from individual cells
f Centroid distribution illustrating the apoptosis induction and proliferation inhibition efficacy of Knock-combos containing specific siRNA
g Heatmap showing the apoptosis induction and proliferation inhibition efficacy for Knock-combos containing specific siRNA
The color index indicates the Z-score normalized phenotype quantification
the data was analyzed using unpaired one-way ANOVA; for panel (d
the data was analyzed using non-parametric Mann–Whitney test
the black dots indicate an overlay of individual data points
the whisker limit is 1.5 times the interquartile range
due to the existence of complex signal transduction networks that are likely to be complementary or parallel and compensate for the single-gene silencing effects
the use of siRNA cocktails targeting multiple disease-related pathways represents an attractive and robust approach to develop siRNA-based therapeutics
emphasizing the critical role of inhibiting Cyclin D1 in the construction of effective siRNA cocktails as potential anti-cancer therapeutics
a A set of 20 siRNAs targeting 6 different cellular pathways: membrane interaction (5 siRNAs)
The screening space (1350) is composed of 20 1-siRNA
b Phenotypic analysis of apoptosis induction for all the tested 1-siRNA (blue)
2-siRNA (red) and 3-siRNA (yellow) Knock-combos
Data were collected from more than 20 cells for each of the 1315 Knock-combos
c Boxplots with scattered data points showing the comparison of the efficacy on apoptosis induction for combinatorial targeting of single
d K-means clustering analysis of all the Knock-combos reveals two distinct clusters in the UMAP space
e Boxplots showing the comparison of apoptosis induction for the 2 identified Knock-combo clusters
f Enrichment analysis of the 20 siRNA targets in each identified Knock-combo clusters
g An interaction network showing the synergic co-operation in apoptosis induction for the 20 siRNAs to different gene targets
where the line color and thickness indicate the phenotypic efficacy of the corresponding combination
The black dots indicate an overlay of individual data points
HER2 or Cyclin D1 showed the most connections to other genes
suggesting the important contributions from siRNAs targeting supplementary genes
uPAR gene appeared to be the best silencing partner for many leading siRNA targeting either survivin or HER2
These screening results provide valuable insights into the construction of combinatorial siRNAs therapeutics for anti-tumor purpose
Since the discovery of RNAi and the demonstration of siRNA in post-transcriptional gene silencing
there has been tremendous interest and effort in harnessing siRNAs for biomedical research and drug development
One of the major issues is that effective gene silencing by siRNA is often hindered by the presence of complementary or parallel signal transduction pathways
which may counteract the action of a single siRNA and substantially offset the therapeutic silencing effects
the use of cocktail siRNAs has been suggested as a feasible and promising drug discovery route
the identification of the most safe and efficient siRNA combination remains challenging and a crucial bottleneck
This study aims to address the problem by developing a high-throughput technology for screening siRNA-based cocktail therapeutics
we believe that the most meaningful siRNA cocktail screening should be oriented towards Knock-combos consisting of 2 to 3 siRNAs
the total possible Knock-combos would reach 178,433,024
which is already a scale inaccessible to any existing methods
hundreds or even thousands of siRNA cocktail formulations could be assayed in just a single well of cell culture
which would be tremendously useful for accelerating the development of siRNA-based therapeutics
Such benefits are not just limited to reducing the time and cost associated with siRNA screening by power of magnitude
but also rely on the capability to answer fundamental siRNA questions that are not addressable by existing methods
such as: (1) whether multiplexed gene silencing are more efficient than single target knockdown; (2) whether a combination of different signaling pathways related siRNAs are more efficient than multiple siRNAs targeting a single pathway; (3) which siRNAs are the most important elements in constructing an effective siRNA cocktail; (4) what is the optimal combination of siRNAs (precise and concise) to achieve the best synergic therapeutic gene-silence
The answers to these fundamental questions could be extensively explored by machine learning and bioinformatic analysis of the large number of single-cell gene silencing data enabled by the scCode-fection technology
as we have demonstrated in the screening of more than 1300 siRNA combinations concerning 20 genes in seeking the most effective cocktail for potential inhibition of cancer cell growth
We believe this study will lead to paths to a systematic and high-throughput platform that would be greatly useful to accelerate further development of siRNA-based therapeutics and enhance their clinical adoption
The fabrication is based on two processes: Connection of Fe3O4-NH2 with gold nanorods through glutaraldehyde and positive coating of PDDA
20 μL stock solution of Fe3O4-NH2 (Invitrogen Thermo Fisher
2 × 109 beads/mL) were incubated in 15% Glutaraldehyde aqueous solution (Sigma-Aldrich) at room temperature on a lab rotator (DLAB
the beads were incubated with 100 μL of Au-NH2 solution (Sigma-Aldrich
1μm in length) while rotating on a lab rotator (DLAB
the assemblies were collected with a magnetic field and blocked with 3% bovine serum albumin (BSA) for 2 h
1 μL NHS-Alexa-514 (Thermo Fisher) was added to Fe3O4-Au assemblies and rotated at 30 rpm (DLAB
MX-RD-Pro) for 2 h followed by three rinses with deionized water
Other codes were prepared in a similar way using a different mixture of the three fluorescent dyes
PDDA was coated for loading negative charged RNAs
Fe3O4-Au assemblies were washed twice with deionized water and then resuspended in 200 μL of 15% (v/v) PDDA solution (Sigma Aldrich)
The suspension was sonicated in a bath for 10 min
The Knock-beads were then washed three times with deionized water and resuspended in 100 μL of PBS for storage
and Fe3O4-Au-PDDA was determined using a Particle Size Analyzer (Zeta sizer
a 20 μL solution of each particle type (Fe3O4
and Fe3O4-Au-PDDA) was added to 500 μL of deionized water
The Particle Size Analyzer was set to detect the size by selecting water as the detection solution and the zeta size mode
with the only difference being the selection of the zeta potential mode
To determine the RNA loading efficiency of Knock-beads
we utilized fluorescence detection of unbound RNA-cy5
the Knock-beads were incubated with RNA-cy5 in deionized water rotating at 30 rpm at room temperature
The mixture was then subjected to a magnetic field
ensuring that the beads were attracted to the side of the tube
The supernatant was then carefully collected
The fluorescence intensity of the supernatant was measured using MD SpectraMax M5e microplate reader
The RNA loading efficiency was calculated based on the fluorescence intensity of the supernatant
as well as the initial concentration of RNA-cy5
This procedure was repeated three times to ensure reproducibility and accuracy of the results
Scanning electron microscopy (SEM; Philips FEG SEM XL30) was employed to characterize the morphology of Fe3O4-Au
the Fe3O4-Au assemblies were deposited onto a silicon wafer and allowed to dry overnight
The dried samples were imaged using a scanning electron microscope at a voltage of 10 kV or 20 kV
SEM images were analyzed using ImageJ software to determine the size distribution of the Fe3O4-Au assemblies
The fluorescence images were captured with confocal laser scanning microscope (Leica SP8
the Knock-beads were mounted with an antifade mounting medium and imaged using a confocal laser scanning microscope
and scanning speed were fixed across the microscopy process
Scanning was performed with a 1 μm step size along the Z-axis spanning the whole cell
3D reconstruction was then performed to visualize the relative position of Knock-beads
Confocal microscopic images were analyzed using ImageJ software to determine the fluorescence labeling and distribution of Knock-beads
For data collection from a screening, imaging-based decoding was performed according to the spectrum encoding (Supplementary Table 5)
The excitation of the 4 quantum dots (emission peak at 547 nm
The emission window was set to be 10 nm wide
we employed the navigator model of Leica Microsystems to capture over 200 tiles from a single culture dish for large area coverage
The resulting large-scale tiles were merged using Leica software to ensure smooth calibration along each edge of the view arrays
A549 (CRM-CCL-185 from American Type Culture Collection
Duke Kunshan University) cells were cultured in Dulbecco’s Modified Eagle Medium (DMEM) supplemented with 10% fetal bovine serum (FBS) and 1% penicillin-streptomycin at 37 °C in a humidified atmosphere containing 5% CO2
and cells were subcultured at 80–90% confluency using Trypsin-EDTA
containing 1 × 107 beads/mL in 2 mL of PBS
was subjected to laser irradiation using a 980 nm laser with a power density of 0.6 W/cm2 and pulse width of 16 μs
Infrared photography was recorded using an infrared camera (Nikon)
Cell viability was tested by adding 5 × 104 beads to A549 cells in a 24-well plate (1 × 105 cells per well)
followed by irradiation with a 0.6 W/cm2 in 16 μs pulse width laser for 2
1 mg/mL) was added and incubated for further 4 h
The MTT-containing medium was then removed
and the formazan crystals were dissolved in dimethyl sulfoxide (DMSO)
The absorbance of each well was measured at 570 nm using Molecular Devices SpectraMax M5e Microplate Reader
The viability of the cells was expressed as the percentage of the absorbance relative to the control group
The Knock-beads were used to deliver fluorescence RNA into A549 using photoporation under a magnetic field
cells were seeded in glass bottom plates at a density of 1 × 106 cells/plate and allowed to adhere overnight
The cells were then incubated with the Knock-beads at a concentration of 4 × 105 for 30 s to allow for absorption of the beads after discharged medium
The cells were then irradiated with a 980-nm laser (16 μs pulse width) for 8 s at a power of 0.6 W/cm2 within a magnetic field
the cells were washed 2 times with PBS within a magnetic field
The efficiency of RNA delivery was determined by visualizing the cells under a confocal microscope and analyzing the uptake of the fluorescence dye with ImageJ
Actin and tubulin were stained for evaluation of the single cell gene knockdown efficiency
TUNEL and Edu were stained to evaluate the anti-tumor efficiency of related Knock-combo
cells were washed with PBS and fixed with 4% paraformaldehyde (Thermo) at room temperature for 30 min
cells were incubated in triton X-100 (0.1% in PBS) at room temperature for 10 min and then rinsed with PBS
2 μL of Actin-Tracker (Actin-tracker kit from Beyotime) were added to each dish and incubated in the dark at room temperature for 60 min
2 μL of Tubulin-tracker (Tubulin-tracker kit from Beyotime) were added to each dish and incubated in the dark for 60 min
One Step TUNEL Apoptosis Assay Kit from Beyotime was used 20 h after photoporation
Terminal Deoxynucleotidyl Transferase (TdT) and fluorescein-dUTP were added to each dish
and cells were incubated at 37 °C for 1 h in the dark allowing for TdT-mediated dUTP Nick-End labeling
BeyoClick™ EdU Cell Proliferation Kit from Beyotime was used
5-ethynyl-2’-deoxyuridine (EDU) at 10 mM was added to the cells before fixation and permeabilization
and 50 μL of click additive solution were added to each dish
followed by a 30-minute incubation in dark at room temperature
the images were first loaded into the Python-based CellPose software
The brightfield channel was used to derive an evaluation of the expected cell diameter in pixels
The grayscale fluorescent channels were then selected for the segmentation processing
The CellPose algorithm was then executed to generate a mask outlining the boundary of individual cells
the cell outlines were exported as an ImageJ ZIP file
which was imported to ImageJ using ROI Manager for further analysis
For the centroid approach in Fig. 6f
the centroid of a specific type of siRNA Knock-combo
denoted as \({{{\boldsymbol{c}}}}_{{{\boldsymbol{s}}}}({x}_{s},\,{y}_{s})\)
refers to the average position of a group of two-dimensional points
For each siRNA combo \(({x}_{i},\,{y}_{i})\)
where \({x}_{i}\) represents the efficacy of apoptosis induction and \({y}_{i}\) represents the efficacy of proliferation inhibition
the centroid for n Knock-combos is obtained by:
For clustering analysis in Fig. 7
The optimal number of clusters (k) was determined using silhouette statistics
The K-Means algorithm was then applied to the preprocessed data with multiple random initializations to find the global optimum for unsupervised derivation of optimal number clusters of the Knock-combos based on the phenotypic features related to cellular apoptosis or proliferation
To prioritize the enrichment of a gene targeted siRNA in the identified Knock-combo clusters (Fig. 7f)
the relative enrichment ratio of each siRNA was calculated using the Z-score normalization defined as:
where X is the appearance frequency of a siRNA for all the Knock-combos in a cluster
μ is the mean appearance frequency of all siRNAs in that cluster
and σ is the standard deviation of the appearance frequency for all siRNAs in the same cluster
The appearance frequency of a siRNA in a cluster is calculated as: counts of Knock-combos containing the siRNA divided by the total number of siRNAs appeared in all Knock-combos of that cluster
To analyze the interaction network and to show the synergic co-operation in apoptosis induction for the siRNAs to their 20 gene targets (Fig. 7g)
The siRNAs were represented as the nodes connected by lines
where the line color and thickness indicate the phenotypic efficacy of the corresponding combination siRNA silencing of the node genes
The line color and thickness were indexed by calculating the mean apoptosis induction among all the Knock-combos containing the two node gene siRNAs (connection score)
A hub score of each node was also derived by taking the sum of all the connections scores for the lines originated from one node
At least three independent biological replicates were used for all experiments
Statistical significance for comparing two experimental conditions is calculated by two-tailed unpaired t test; for comparing one control with multiple experimental conditions
the statistical significance is calculated using the unpaired one-way ANOVA test
unpaired nonparametric Mann–Whitney test is used to compare different groups
A p value less than 0.05 is considered to be statistically significant
and all the p values are indicated in the respective figures
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
The data generated in this study are provided in the Supplementary Information/Source Data file. Source data are provided with this paper
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Splitting of the interband absorption edge in Au
Cellpose: a generalist algorithm for cellular segmentation
Partial depletion of gamma-actin suppresses microtubule dynamics
Unravelling the enigma of siRNA and aptamer mediated therapies against pancreatic cancer
DNA damaging agents and DNA repair: From carcinogenesis to cancer therapy
RNAi-based therapeutics and tumor targeted delivery in cancer
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cancer networks and pathway-directed drug discovery
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MYC protein interactors in gene transcription and cancer
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Size-dependent cytotoxicity of gold nanoparticles
Biocompatibility and cytotoxicity of gold nanoparticles: recent advances in methodologies and regulations
Pulsed electromagnetic fields stimulate osteogenic differentiation in human bone marrow and adipose tissue derived mesenchymal stem cells
Highly multiplexed spatial mapping of microbial communities
Approved HIV reverse transcriptase inhibitors in the past decade
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This work was supported by National Natural Science Foundation of China (U20A20194
P.S.) from the Research Grants Council of Hong Kong SAR
Shenzhen-Hong Kong-Macau Science and Technology Program (Category C
by a Kunshan Shuangchuang Talent Grant (KSSC202102069
Support from Innovation and Technology Commission of Hong Kong through the Center for Cerebro-Cardiovascular Health Engineering and funds from City University of Hong Kong (7005084
These authors contributed equally: Feng Guo
Hong Kong Centre for Cerebro-Cardiovascular Health Engineering
Department of Chemical and Biological Engineering
The Hong Kong University of Science and Technology
Division of Natural and Applied Sciences & Global Health Research Center
Center of Super-Diamond and Advanced Films (COSDAF)
designed the experiments and carried out the investigation
contributed to the validation of siRNA gene silencing
and F.Gao contributed to the informatic analysis of the large-scale screening data
contributed to the writing of the manuscript
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DOI: https://doi.org/10.1038/s41467-024-53419-7
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Therapeutic small interfering RNA (siRNA) requires sugar and backbone modifications to inhibit nuclease degradation
metabolic stabilization by phosphorothioate (PS)
the only backbone chemistry used clinically
may be insufficient for targeting extrahepatic tissues
synthesis and characterization of extended nucleic acid (exNA) consisting of a methylene insertion between the 5′-C and 5′-OH of a nucleoside
exNA incorporation is compatible with common oligonucleotide synthetic protocols and the PS backbone
provides stabilization against 3′ and 5′ exonucleases and is tolerated at multiple oligonucleotide positions
A combined exNA–PS backbone enhances resistance to 3′ exonuclease by ~32-fold over the conventional PS backbone and by >1,000-fold over the natural phosphodiester backbone
The improved efficacy and durability imparted by exNA may enable therapeutic interventions in extrahepatic tissues
both with siRNA and with other oligonucleotides such as CRISPR guide RNA
The data supporting the findings of this study are available from the corresponding authors upon reasonable request. The raw NMR data are included in the Supplementary Information
The chemical evolution of oligonucleotide therapies of clinical utility
Treating disease at the RNA level with oligonucleotides
mechanism and clinical status of antisense oligonucleotides and duplex RNAs
structure and function of approved oligonucleotide therapeutics
Delivery of therapeutic small interfering RNA: the current patent-based landscape
Re-engineering RNA molecules into therapeutic agents
The chemical structure and phosphorothioate content of hydrophobically modified siRNAs impact extrahepatic distribution and efficacy
Overcoming the challenges of tissue delivery for oligonucleotide therapeutics
From bench to bedside: improving the clinical safety of GalNAc–siRNA conjugates using seed-pairing destabilization
Analysis of RNA exonucleolytic activities in cellular extracts
Impact of enhanced metabolic stability on pharmacokinetics and pharmacodynamics of GalNAc–siRNA conjugates
Advanced siRNA designs further improve in vivo performance of GalNAc–siRNA conjugates
Investigating the pharmacodynamic durability of GalNAc–siRNA conjugates
RNA interference using boranophosphate siRNAs: structure–activity relationship
High potency silencing by single-stranded boranophosphate siRNA
Efficient delivery of RNAi prodrugs containing reversible charge-neutralizing phosphotriester backbone modifications
A single amide linkage in the passenger strand suppresses its activity and enhances guide strand targeting of siRNAs
Amide modifications in the seed region of the guide strand improve the on-target specificity of short interfering RNA
Selection of GalNAc-conjugated siRNAs with limited off-target-driven rat hepatotoxicity
The α-(l)-threofuranosyl nucleic acid modification improves stability
and Ago2 binding and mitigates off-target effects of small interfering RNAs
Single-stranded siRNAs activate RNAi in animals
5′-(E)-Vinylphosphonate: a stable phosphate mimic can improve the RNAi activity of siRNA–GalNAc conjugates
siRNA carrying an (E)-vinylphosphonate moiety at the 5′-end of the guide strand augments gene silencing by enhanced binding to human Argonaute-2
5′-Vinylphosphonate improves tissue accumulation and efficacy of conjugated siRNAs in vivo
Structurally constrained phosphonate internucleotide linkage impacts oligonucleotide–enzyme interaction
and modulates siRNA activity and allele specificity
Phosphoryl guanidines: a new type of nucleic acid analogues
Impact of stereopure chimeric backbone chemistries on the potency and durability of gene silencing by RNA interference
essential components of therapeutic oligonucleotides
Structural analysis of human Argonaute-2 bound to a modified siRNA guide
A highly durable RNAi therapeutic inhibitor of PCSK9
Metabolite profiling of the antisense oligonucleotide eluforsen using liquid chromatography–mass spectrometry
Nonclinical pharmacokinetics and absorption
the first approved N-acetylgalactosamine-conjugated RNA interference therapeutic
Use of 5-deoxy-ribo-hexofuranose derivatives for the preparation of 5′-nucleotide phosphonates and homoribonucleosides
Biomimetic modeling of the decomposition of 2′-chloro-2′-deoxynucleotides by ribonucleotide reductases to give 3(2H)-furanones which can effect mechanism-based inactivation by Michael-type alkylation
hybridization and modeling studies of modified oligonucleotides
Khvorova, A., Roux, L. M. & Yamada, K. Modified oligonucleotides with increased stability. US Patent 2020025017-W (2020); https://portal.unifiedpatents.com/patents/patent/WO-2020198509-A3
Khvorova, A., Roux, L. M. & Yamada, K. Synthetic oligonucleotides having regions of block and cluster modifications. US Patent 20210395739A1 (2021); https://patents.google.com/patent/US20210395739A1/en
Khvorova, A., Roux, L. M. & Yamada, K. Synthesis of modified oligonucleotides with increased stability. US Patent 20220010309A1 (2022); https://patents.google.com/patent/US20220010309A1/en
The chemistries and consequences of DNA and RNA methylation and demethylation
Methylation across the central dogma in health and diseases: new therapeutic strategies
Phospho-carboxylic anhydride of a homologated nucleoside leads to primer degradation in the presence of a polymerase
Structural basis of duplex thermodynamic stability and enhanced nuclease resistance of 5′-C-methyl pyrimidine-modified oligonucleotides
β-Cyanoethyl N,N-dialkylamino/N-morpholinomonochloro phosphoramidites
new phosphitylating agents facilitating ease of deprotection and work-up of synthesized oligonucleotides
Modified internucleoside linkages for nuclease-resistant oligonucleotides
The crystal structure of the Argonaute2 PAZ domain reveals an RNA binding motif in RNAi effector complexes
siRNA carrying an (E)-vinylphosphonate moiety at the 5′ end of the guide strand augments gene silencing by enhanced binding to human Argonaute-2
Structural basis for overhang-specific small interfering RNA recognition by the PAZ domain
Hydrophobically modified siRNAs silence Huntingtin mRNA in primary neurons and mouse brain
Comparison of partially and fully chemically-modified siRNA in conjugate-mediated delivery in vivo
Single-molecule imaging reveals that argonaute reshapes the binding properties of its nucleic acid guides
Structure of yeast Argonaute with guide RNA
Helix-7 in Argonaute2 shapes the microRNA seed region for rapid target recognition
siRNA seed region is divided into two functionally different domains in RNA interference in response to 2′-OMe modifications
Functional features defining the efficacy of cholesterol-conjugated
siRNA function in RNAi: a chemical modification analysis
Single modification at position 14 of siRNA strand abolishes its gene-silencing activity by decreasing both RISC loading and target degradation
Target RNA-directed trimming and tailing of small silencing RNAs
Highly complementary target RNAs promote release of guide RNAs from human Argonaute2
Chimeric siRNAs with chemically modified pentofuranose and hexopyranose nucleotides: altritol-nucleotide (ANA) containing GalNAc-siRNA conjugates: in vitro and in vivo RNAi activity and resistance to 5′-exonuclease
Modified deoxyoligonucleotides stable to exonuclease degradation in serum
2′-O-Methyl at 20-mer guide strand 3′ termini may negatively affect target silencing activity of fully chemically modified siRNA
Chemical modification of siRNAs to improve serum stability without loss of efficacy
Diverse lipid conjugates for functional extra-hepatic siRNA delivery in vivo
Roehl, I., Schuster, M. & Seiffert, S. Oligonucleotide detection method. US Patent 20110201006-A1 (2011); https://portal.unifiedpatents.com/patents/patent/US-20110201006-A1
A divalent siRNA chemical scaffold for potent and sustained modulation of gene expression throughout the central nervous system
Selective striatal neuronal loss in a YAC128 mouse model of Huntington disease
Structures of human exonuclease 1 DNA complexes suggest a unified mechanism for nuclease family
Coupled 5′ nucleotide recognition and processivity in Xrn1-mediated mRNA decay
Structural principles for the inhibition of the 3′–5′ exonuclease activity of Escherichia coli DNA polymerase I by phosphorothioates
Overcoming cellular barriers for RNA therapeutics
GalNAc-siRNA conjugates: leading the way for delivery of RNAi therapeutics
Utilization of unlocked nucleic acid (UNA) to enhance siRNA performance in vitro and in vivo
Allele-selective inhibition of expression of huntingtin and ataxin-3 by RNA duplexes containing unlocked nucleic acid substitutions
RNA-based therapeutics: an overview and prospectus
tRNA therapeutics burst onto startup scene
Applications of CRISPR technologies in research and beyond
Mesyl phosphoramidate backbone modified antisense oligonucleotides targeting miR-21 with enhanced in vivo therapeutic potency
Synthesis and evaluation of parenchymal retention and efficacy of a metabolically stable O-phosphocholine-N-docosahexaenoyl-l-serine siRNA conjugate in mouse brain
Removal of t-butyldimethylsilyl protection in RNA-synthesis
3HF) is a more reliable alternative to tetrabutylammonium fluoride (TBAF)
Pharmacokinetic profiling of conjugated therapeutic oligonucleotides: a high-throughput method based upon serial blood microsampling coupled to peptide nucleic acid hybridization assay
A high-throughput method for direct detection of therapeutic oligonucleotide-induced gene silencing in vivo
Improved pharmacokinetic and bioavailability support of drug discovery using serial blood sampling in mice
Chemical engineering of therapeutic siRNAs for allele-specific gene silencing in Huntington’s disease models
Huntingtin is a cytoplasmic protein associated with vesicles in human and rat brain neurons
glmmTMB balances speed and flexibility among packages for zero-inflated generalized linear mixed modeling
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Ali for maintaining the infrastructure for nuclear magnetic resonance (NMR) and Y
Nguyen for measurement of high-resolution mass analysis
University of Massachusetts Chan Medical School
Harvard Medical School and Mass General Institute for Neurodegenerative Disease
contributed to the experimental design for exNA studies in hepatic and extrahepatic tissues
contributed to the experimental design for exNA studies in CNS
contributed to the exNA thermal stability and nuclease resistance study
contributed to the oligonucleotide synthesis
contributed to the statistical analysis of exNA CNS studies
gave inspirational intellectual contributions
have filed patent applications for exNA platforms
discloses ownership of stocks in RXi Pharmaceuticals and Advirna
and is a founder of Atalanta Therapeutics and Comanche Biopharma
is an employee of Comanche Biopharma and owns stock options
The remaining authors declare no competing interests
Nature Biotechnology thanks Eriks Rozners and the other
Scheme 1 and Data (synthetic oligonucleotide sequence information
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DOI: https://doi.org/10.1038/s41587-024-02336-7
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aberrant RNAs produced by endogenous genes or transgenes are normally degraded by the nuclear and cytosolic RNA quality control (RQC) pathways
and aberrant RNAs are converted into siRNAs that initiate post-transcriptional gene silencing (PTGS) in the cytosol
How aberrant RNAs are selected and brought to the cytoplasm is not known
Here we show that the RNA-binding protein SUPPRESSOR OF GENE SILENCING (SGS)3 shuttles between the cytosol and the nucleus where it associates with the ISWI-like CHROMATIN REMODELER (CHR)11 and with RNAs transcribed from PTGS-sensitive transgene loci binding CHR11
Knocking down CHR11 and its paralog CHR17 strongly reduces transgene PTGS
suggesting that SGS3 recruitment by CHR11/17 facilitates PTGS initiation
CHR11 is also enriched at endogenous protein-coding genes (PCGs) producing nat-siRNAs and va-siRNAs under biotic or abiotic stresses
and this production is reduced in chr11 chr17 double mutants at genome-wide level
impairing CHR11 and CHR17 rescues the lethal phenotype caused by the massive production of siRNAs from PCGs in RQC-deficient mutants
We propose that SGS3 recruitment by CHR11/17 allows exporting RNAs to the cytosol to initiate the production of siRNAs
This suggests that viral RNAs bound to AGO1 and protected by SGS3 are transformed into dsRNA by RDR6
thus creating an amplification loop that increases the production of siRNAs and further contributes to decreasing virus titer
these results indicate that many types of endogenous or exogenous genes can produce siRNAs after the transformation of abRNA into dsRNA by RDR6
major questions remain unanswered regarding the way abRNAs are selectively exported to the cytosol for transformation into dsRNA by RDR6
we show that transgenes and endogenous genes that produce siRNAs bind to the ISWI-like CHROMATIN REMODELER (CHR)11
We show that CHR11 and its paralog CHR17 interact with the RNA-binding protein SGS3 and that SGS3 shuttles between cytosol and the nucleus where it binds transgene RNAs
We propose a model where CHR11/CHR17 and SGS3 are major nuclear determinants promoting the initiation of siRNA production
a SGS3 and CHR11 structures. CHR11 and SGS3 domains interacting in yeast two-hybrid are shown in gray. The sequence of the CHR11 clone retrieved in the in yeast two-hybrid screen is shown in Supplementary Fig. 1
b Localization of CHR11 full-length and truncated forms (stop1 and stop2) in N
benthamiana (the same results were obtained twice in N
The overlay is shown for DAPI/YFP/chlorophyll fluorescences
c BiFC Interaction between SGS3 and CHR11 (full-length and truncated forms) in the nucleus of N
Subcellular localization of reconstructed YFP was determined in the leaf epidermis for SGS3 protein in fusion with the C- terminal part of YFP (YC) and CHR11 proteins in fusion with the N- terminal part of YFP (YN)
The overlay is shown for DAPI/YFP/chlorophyll fluorescences (the same results were obtained 4 times in N
d SGS3 is associated with fractions enriched in microsomal and nuclear compartments in wild-type Arabidopsis
and in the chr11 chr17 double mutant complemented with the p35S:FLAG-CHR11construct (the same results were obtained twice on two different subcellular fractionations)
The sgs3-1 null allele is used as a negative control
suggesting a dual localization of SGS3 in the nucleus and cytosol of Arabidopsis cells
c Nuclear localization of a control line expressing GFP-CHR11 under the 35S promoter (the same results were obtained more than twice in A
resides in the same cytosolic siRNA bodies
these results clearly indicate that only SGS3 shuttles between the nuclear and cytosolic compartments
and dissociates before SGS3 re-export to the cytosol
no report to date has established a link between the ISWI complex and PTGS
GUS siRNA and amiRCHR11-17 accumulation at 18 days in the progeny of lines L1/ pUBQ10:amirCHR11-17 lines #125 and #135 harvested in bulk
GUS activity is given below for each sample used for RNA extraction (the results are shown for the northern blot obtained from one unique extraction of each sample)
indicating that impairment of CHR11/17 does not modify the level of transcription of the p35S:GUS transgene
these results suggest that the reason why CHR11/17 impairment affects S-PTGS is not due to changes in the level of transcription of transgene mRNA
it remains possible that transgene transcription is qualitatively affected
modifying the ratio between functional mRNAs and aberrant RNAs
ChIP-qPCR analyses were performed on 15-day-old seedlings of the indicated genotypes
a ChIP was performed on the L1/pUBQ10:GFP-CHR11 line using GFP antibodies for IP
Graphical representation shows the fold change of two biological repeats
b ChIP was performed on the L1/pUBQ10:FLAG-CHR11 using Flag antibodies for IP
which expressed CHR11 at a similar level than in L1/pUBQ10:FLAG-CHR11
Graphical representation shows the fold change as the mean of three biological repeats and displays every data point
Error bars represent the standard deviation
In addition to validating the 6b4 locus as a control
this result supports the hypothesis that the 6b4 locus triggers S-PTGS in an RQC-deficient background through CHR11/SGS3 selection/recruitment
these results suggest that CHR11/17 generally promotes transgene S-PTGS by binding to transgene loci
thus allowing the association of transgene RNAs with SGS3 in the nucleus and their export to the cytosol to initiate S-PTGS
indicating that the added NLS is functional and that the export of the SGS3-NLS-GFP protein from the nucleus to the cytosol is inhibited or strongly diminished at 38 °C
RIP analysis of GUS mRNA associated with SGS3 was performed using L1/sgs3 plants complemented by pRDR6:SGS3-NLS-GFP
and L1 line (without TAG) as control for normalization
RT-qPCR was performed to determine the accumulation levels of 5’ terminal part
qPCR Fold enrichment of the immunoprecipitated (IP) was calculated as 2exp(−ΔΔCt [RIP in SGS3-NLS-GFP line/background in L1])
Fold enrichment of the qPCR internal control
PP2A was also calculated and arbitrarily set to 1
The mean values and standard deviation of three independent experiments are shown as every data point
The results presented above suggest a model in which SGS3 is recruited by CHR11 and presumably its paralog CHR17 to transgene DNA
allowing certain nascent transgene RNAs to bind SGS3
SGS3 shuttling between nucleus and cytosol likely promotes the export of SGS3-bound transgene RNAs to the cytosol where they can be fully converted to dsRNA by RDR6 in siRNA bodies
c Variation of 21/22nt ta-siRNA accumulation between chr11 chr17 and Col-0
Values are log2 fold changes according to DESeq2 differential analysis (n = 3 biologically independent samples per genotype and 7 ta-siRNA genes)
The median is represented by the horizontal line
the box indicates the interquartile range (IQR
and black points indicate points outside this range
d Accumulation of va-siRNAs upon TCV infection of Col-0 and chr11 chr17
Values are log2 fold changes according to DESeq2 differential analysis compared to Mock treatment (n = 3 biologically independent samples per genotype and condition
The number shown above indicates the p-values of the difference of log2 fold change determined by a Wilcoxon test (the value displayed “< 2.2e-16” is the smallest p-value R will return for a Wilcoxon test)
e Variation of va-siRNAs upon TCV infection of Col-0 and chr11 chr17
Values of the heat map are log2 fold changes according to DESeq2 differential analysis compared to Mock treatment
these results support the relevance of CHR11 in the production of siRNAs from PCGs
Pictures of representative plants of the indicated genotypes grown for 27 days in short days
When the genomic arrangement allows the production of sense and antisense RNAs forming dsRNA with a 5’ overhang
which probably releases the CHR11-SGS3 interaction
RNAs bound to SGS3 are converted to dsRNA by RDR6
followed by processing by DCL4 and DCL2 into 21-nt siRNAs that can execute PTGS and 22-nt siRNAs that allow PTGS amplification
The model described for the p35S-GUS transgene locus likely applies for endogenous PCG/NAT pairs
(This figure was entirely created by authors using ppt)
the native SGS3 shuttles between cytosol and nucleus
When nucleo-cytosolic export is not inhibited
except when CHR11 level is increased in the nucleus
or when SGS3 fused to a canonical NLS is forced to remain in the nucleus after heat stress
suggesting that SGS3 is actively exported from the nucleus to the cytosol
together with the RNA binding and protecting effect of SGS3 against degradation by RQC
certainly contributes to addressing transgene RNAs to the cytosol to initiate PTGS
Following cleavage at the polyadenylation site of the NPT transcript
the downstream part of the read-through transcript
SGS3 could then bind to the GUS/SUG duplex in the nuclei because it has a 5’ overhang
the native AGO1 protein produced in the cytosol has an exposed NLS and a buried NES
allowing the AGO1/miRNA complexes to be exported to the cytosol
The binding of SGS3 to dsRNA and/or the dissociation of SGS3 from CHR11 may also expose its NES
allowing the SGS3-dsRNA complex to be exported to the cytosol
the SGS3-bound GUS/SUG duplex could be processed into 21- and 22-nt siRNAs by DCL4 and DCL2 to initiate PTGS
GUS and/or SUG RNAs could also be separately transformed into dsRNA by RDR6 prior to DCL2/DCL4-mediated processing into 21- and 22-nt siRNAs
after which the total aerial parts of 4 to 12 plants were harvested
pRDR6:SGS3-NLS-GFP was obtained by cloning canonical NLS sequences in speI of SGS3-pDONR207 prior to recombination in the compatible destination vector pRDR6-PGWB4
and pUBC‐GFP-DEST to make pUBQ10-GFP-CHR11
pUBQ10:Flag-CHR11 was obtained by cloning in pDONR207 CHR11 cDNA amplified by attB1FlagCHR11F and attB2CHR11Rbis primers prior to recombination in the compatible destination vector pUB-DEST
France) PCR‐based mutagenesis was used to introduce premature stop1 and stop2 in CHR11 cloned in pDONR207 using CHR11stop1Fbis /CHR11stop1Rbis and CHR11stop2F/CHR11stop2R pairs of primers to obtained p35S:GFP-CHR11stop1 and stop2
AmiRCHR11-17 was synthesized and cloned in pUC57 by GenScript Corporation (New Jersey 08854-3900)
Primers amiRf and amiRr were used to amplified amiRCHR11-17 in its precursor backbone for cloning in the pDONR207 vector prior to recombination in the compatible destination vector pUB-Dest to obtained pUBQ10:amirCHR11-17
CDS of RDR6 without its stop codon was cloned in SalI and NotI of pENTR1A vector after amplification by the primers pairs RDR6f/RDR6r (Supplementary Table 3) prior recombination in the compatible destination vector pH7FWG2 to obtained p35S:RDR6-GFP
64 were LacZ + (2 clones issued from screen without expression
A fraction of the yeast plasmid minipreparation from each His + /LacZ + clone was used to transform HB101 E
coli clones was transformed again into either the L40 strain carrying LexA/SGS3 to confirm interaction or an L40 carrying an unrelated hybrid protein
Only 37 His + /LacZ+ clones were specific for LexA/SGS3 and in frame with the GAL4 sequence
28 interact with the C‐terminal three coiled‐coil domains of SGS3
which included the two clones recovered on a selective medium without expression (suggesting a strong interaction between the two partners)
One of these two clones corresponded to the C-terminal part of CHR11
Samples were excited with a 514 nm argon laser (50%) with an emission band of 520–550 nm for YFP detection and 640–700 nm for chlorophyll autofluorescence
Arabidopsis roots were directly imaged on a Leica TCS-SP5 (Leica Microsystems) equipped with a photomultiplier tube and hybrid detectors with an HCX PL APO CS 20.0 × 0.70 IMM objective
GFP was imaged with 488 nm excitation using an Argon laser
For the nuclear export inhibition experiment
five days-old seedlings were transferred to 100ul liquid MS-medium with Leptomycin B (Sigma LMB
at 5 uM final concentration corresponding to methanol at 4.7% final) and incubated 28 h before imaging
Controls were incubated 28H in 100 ul liquid MS-medium with methanol added at 4.7% final
Two grams of rosette leaves of 31 days-old plants were ground in 16 ml buffer supplemented with 1.14 M sucrose (10 mM Tris–HCl pH 7.5
1 mM DTT and protease inhibitor cocktail sigma p9599)
The sample was filtered through Miracloth and centrifuged at 1000 × g for 10 min at 4 °C
Supernatants recovered after the first centrifugation was supplemented with 0.15% Triton X100 and was centrifuged at 100,000 × g 45 min at 4 °C to obtain the microsomal fractions (pellet)
The first pellet was washed twice with 10 ml buffer (10 mM Tris–HCl pH 7.5
and protease inhibitor cocktail sigma p9599) supplemented with 0.15% Triton X100
The last pellet corresponding to the nuclear fraction was resuspend in lysis buffer (10 mM Tris–HCl pH 7
and protease inhibitor cocktail sigma p9599) and sonicate on bioruptor
Protein concentration was quantified using a detergent-compatible BCA kit (Bio-Rad)
and 50 μg of protein were loaded on 8% SDS PAGE
Proteins were electroblotted onto nitrocellulose membranes (Amersham Hybond ECL)
The membrane was blocked in 5% non-fat dry milk in 1 × TBSTT (0.25% Tween-20
and incubated with primary antibody in 5% non-fat dry milk and 1 × TBST for 1 h at room temperature
The membrane was then rinsed in 1 × TBST for 20 min before incubation with HRP-coupled secondary IgGs
Antigens were detected using chemiluminescence for HRP immunoblot (Amersham ECL Plus)
The antibodies used were anti-SGS3 (ref B152 from Santacruz
1/200e dilution) anti-H3 (ab1791 from Abcam
followed by sonication using Covaris S220 ultrasonicator 12 min with 5% duty cycle
30 μL of GFP-trap-M beads (gfm-20/500 ul chromotech) was washed twice and resuspended in 60 μL of ChIP dilution buffer
60 μL of magnetic beads G was washed twice and resuspended in 60 μL of ChIP dilution buffer
5 μL of anti-FLAG M2 clone SIGMA(F3165) were added to the beads G and incubated for at least 3 h at 4 °C with gentle rotation on a wheel
After three washes the beads plus antibodies were resuspended in 100 μL of ChIP dilution buffer
1 mL of the chromatin solution was added to the antibodies plus beads (GFP-trap-M or G beads plus anti-Flag) and was incubated overnight at 4 °C with gentle rotation for GFP or Flag capture
the reverse crosslinking (5 h at 65 °C) and elution were performed using an IPure kit (Diagenode)
and the chromatin was stored at − 20 °C until analysis
Here control is L1 for ChIP on L1/pUBQ10:GFP-CHR11 and L1/ pUBQ10:GFP-CHR11 for ChIP on L1/pUBQ10:Flag-CHR11
sample is our target and internal reference is GAPDH
Two to four biological replicates were analyzed each time
Results show the mean and SD of the independent biological replicates
Fold enrichment in the immunoprecipitated fraction (IP) compared to input fraction was calculated as 2exp(−ΔΔCt [RIP in SGS3-NLS-GFP line/RIP background in L1 line])
which correspond to ratio between percentage of input calculated for SGS3-NLS-GFP line / L1 control line
Fold enrichment was calculated for the GUS mRNA target
Mean values and standard errors of three independent experiments are shown
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
and activities of endogenous silencing small RNAs in Arabidopsis
3’ fragment of miR173-programmed RISC-cleaved RNA is protected from degradation in a complex with RISC and SGS3
A pathway for the biogenesis of trans-acting siRNAs in Arabidopsis
Heat stress promotes Arabidopsis AGO1 phase separation and association with stress granule components
A neomorphic sgs3 allele stabilizing miRNA cleavage products reveals that SGS3 acts as a homodimer
Cytoplasmic Arabidopsis AGO7 accumulates in membrane-associated siRNA bodies and is required for ta-siRNA biogenesis
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decapping prevents RDR6-dependent production of small interfering RNAs from endogenous mRNAs
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Ribosome stalling and SGS3 phase separation prime the epigenetic silencing of transposons
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a chromatin-remodeling factor essential for nuclear proliferation during female gametogenesis in Arabidopsis thaliana
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and XRN3 are endogenous RNA silencing suppressors
The Zinc-Finger Protein SOP1 Is Required for a Subset of the Nuclear Exosome Functions in Arabidopsis
The RNA helicases AtMTR4 and HEN2 target specific subsets of nuclear transcripts for degradation by the nuclear exosome in Arabidopsis thaliana
Second-site mutagenesis of a hypomorphic argonaute1 allele identifies SUPERKILLER3 as an endogenous suppressor of transgene posttranscriptional gene silencing
ISWI proteins participate in the genome-wide nucleosome distribution in Arabidopsis
A SWI/SNF chromatin-remodeling complex acts in noncoding RNA-mediated transcriptional silencing
Analysis of mRNA-derived siRNAs in mutants of mRNA maturation and surveillance pathways in Arabidopsis thaliana
Hua, X. et al. Global analysis of RNA-dependent RNA polymerase-dependent small RNAs reveals new substrates and functions for these proteins and SGS3 in arabidopsis. Noncoding RNA 7, https://doi.org/10.3390/ncrna7020028 (2021)
dsRNA with 5’ overhangs contributes to endogenous and antiviral RNA silencing pathways in plants
Nucleo-cytosolic shuttling of ARGONAUTE1 prompts a revised model of the plant microRNA pathway
A branched pathway for transgene-induced RNA silencing in plants
Arabidopsis mutants impaired in cosuppression
The conserved RNA trafficking proteins HPR1 and TEX1 are involved in the production of endogenous and exogenous small interfering RNA in Arabidopsis
Arabidopsis SGS2 and SGS3 genes are required for posttranscriptional gene silencing and natural virus resistance
AtXRN4 degrades mRNA in Arabidopsis and its substrates include selected miRNA targets
Improved Gateway binary vectors: high-performance vectors for creation of fusion constructs in transgenic analysis of plants
A ubiquitin-10 promoter-based vector set for fluorescent protein tagging facilitates temporal stability and native protein distribution in transient and stable expression studies
Highly specific gene silencing by artificial microRNAs in Arabidopsis
sgs1: a neomorphic nac52 allele impairing post-transcriptional gene silencing through SGS3 downregulation
Protein-protein interactions among the Aux/IAA proteins
Cloning of Rac and Rho-GDI from tobacco using an heterologous two-hybrid screen
Mutations in the Arabidopsis H3K4me2/3 demethylase JMJ14 suppress posttranscriptional gene silencing by decreasing transgene transcription
Genome-wide identification of RETINOBLASTOMA RELATED 1 binding sites in Arabidopsis reveals novel DNA damage regulators
Profiling histone modification patterns in plants using genomic tiling microarrays
Genome-wide identification and testing of superior reference genes for transcript normalization in Arabidopsis
Contrasting epigenetic control of transgenes and endogenous genes promotes post-transcriptional transgene silencing in Arabidopsis
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We thank Hervé Ferry and Philippe Maréchal for taking care of the plants
We thank François Roudier and Jerémie Bazin for the discussion and advices respectively
on the ChIP protocol adapted for chromatin remodeler proteins and on the RIP protocol
We also thank Martin Lacroix for fruitful discussions
Research in the Vaucheret laboratory is supported by grants from the French Agence Nationale pour la Recherche (ANR-16-CE12-0032 and ANR-20-CE12-0009)
The IJPB benefits from the support of the LabEx Saclay Plant Sciences-SPS (ANR-17-EUR-007)
This work has benefited from the support of IJPB’s Plant Observatory technological platforms
Institut Jean-Pierre Bourgin for Plant Sciences (IJPB)
analyzed the data and wrote the manuscript
Nature Communications thanks Yuichiro Watanabe
and the other anonymous reviewer(s) for their contribution to the peer review of this work
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DOI: https://doi.org/10.1038/s41467-025-57394-5
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Strategies to enhance the anti-tumor immune response of stereotactic ablative radiotherapy (SABR) at primary tumors and abscopal sites are under intensive investigation
Here we report a metabolizable binary supracluster (BSCgal) that combines gold nanoclusters as radiosensitizing adjuvants with small interfering RNA (siRNA) targeting the immunosuppressive mediator galectin-1 (Gal-1)
BSCgal comprises reversibly crosslinked cationic gold nanoclusters and siRNA complexes in a polymer matrix that biodegrades over weeks
facilitating clearance (90.3% in vivo clearance at 4 weeks) to reduce toxicity
The particle size well above the renal filtration threshold facilitates passive delivery to tumors
Using mouse models of head and neck cancer
we show that BSCgal augments the radiodynamic and immunotherapeutic effects of SABR at the primary and metastatic tumors by promoting tumor-inhibitory leukocytes
upregulating cytotoxic granzyme B and reducing immunosuppressive cell populations
It outperforms SABR plus Gal-1 antagonists
chemoradiation drug cisplatin or PD-1 inhibitor
This work presents a translatable strategy to converge focal radiosensitization with targeted immune checkpoint silencing for personalized radioimmunotherapy
Integrated MRI-guided radiotherapy—opportunities and challenges
Image-guided radiotherapy: from current concept to future perspectives
Immunotherapy and stereotactic ablative radiotherapy (ISABR): a curative approach
Patterns of disease recurrence after stereotactic ablative radiotherapy for early stage non-small-cell lung cancer: a retrospective analysis
Individualized adaptive stereotactic body radiotherapy for liver tumors in patients at high risk for liver damage: a phase 2 clinical trial
and patterns of failure after single-fraction stereotactic body radiation therapy (SBRT) for oligometastases
Long-term follow-up and patterns of recurrence of patients with oligometastatic NSCLC treated with pulmonary SBRT
The role of stereotactic ablative body radiotherapy in renal cell carcinoma
Radiotherapy and immunotherapy: a beneficial liaison
Stereotactic radiotherapy and pembrolizumab for oligometastatic renal tumors: the RAPPORT trial
Randomized phase II trial of nivolumab with stereotactic body radiotherapy versus nivolumab alone in metastatic head and neck squamous cell carcinoma
NRG-GU012: randomized phase II stereotactic ablative radiation therapy (SABR) for patients with metastatic unresected renal cell carcinoma (RCC) receiving immunotherapy (SAMURAI)
The oligometastatic spectrum in the era of improved detection and modern systemic therapy
Gold nanoparticles for applications in cancer radiotherapy: mechanisms and recent advancements
Low-dose X-ray radiotherapy–radiodynamic therapy via nanoscale metal–organic frameworks enhances checkpoint blockade immunotherapy
Synergistic checkpoint-blockade and radiotherapy–radiodynamic therapy via an immunomodulatory nanoscale metal–organic framework
First-in-human study testing a new radioenhancer using nanoparticles (NBTXR3) activated by radiation therapy in patients with locally advanced soft tissue sarcomas
NBTXR3 crystalline nanoparticles and radiation therapy in treating randomized patients in two arms with soft tissue sarcoma of the extremity and trunk wall. https://clinicaltrials.gov/study/NCT02379845
Advanced multimodal nanoparticles delay tumor progression with clinical radiation therapy
AGuIX® from bench to bedside—transfer of an ultrasmall theranostic gadolinium-based nanoparticle to clinical medicine
Radiosensitization of multiple brain metastases using AGuIX gadolinium based nanoparticles (NANO-RAD). https://clinicaltrials.gov/study/NCT02820454
Radiosensitization by gold nanoparticles: will they ever make it to the clinic
Critical parameters to translate gold nanoparticles as radiosensitizing agents into the clinic
Renal clearable catalytic gold nanoclusters for in vivo disease monitoring
Glutathione-mediated biotransformation in the liver modulates nanoparticle transport
Proximal tubules eliminate endocytosed gold nanoparticles through an organelle-extrusion-mediated self-renewal mechanism
Glomerular barrier behaves as an atomically precise bandpass filter in a sub-nanometre regime
Intratumoral biosynthesis of gold nanoclusters by pancreatic cancer to overcome delivery barriers to radiosensitization
Targeted gold nanocluster-enhanced radiotherapy of prostate cancer
Atomically precise gold–levonorgestrel nanocluster as a radiosensitizer for enhanced cancer therapy
Surface functionalization of gold nanoclusters with arginine: a trade-off between microtumor uptake and radiotherapy enhancement
Unraveling galectin-1 as a novel therapeutic target for cancer
Prognostic significance of galectin-1 expression in patients with cancer: a meta-analysis
Galectin-1 is a poor prognostic factor in patients with glioblastoma multiforme after radiotherapy
Targeting galectin-driven regulatory circuits in cancer and fibrosis
Galectin-1: a link between tumor hypoxia and tumor immune privilege
Galectins as modulators of tumour progression
Turning ‘sweet’ on immunity: galectin–glycan interactions in immune tolerance and inflammation
Galectin-1 research in T cell immunity: past
Galectin-1–driven T cell exclusion in the tumor endothelium promotes immunotherapy resistance
Galectin-1 mediates chronic STING activation in tumors to promote metastasis through MDSC recruitment
Enhanced anticancer efficacy by ATP-mediated liposomal drug delivery
From aggregation-induced emission of Au(I)–thiolate complexes to ultrabright Au(0)@Au(I)–thiolate core–shell nanoclusters
Protamine-induced condensation and decondensation of the same DNA molecule
Disulfide-cross-linked PEG-poly(amino acid)s copolymer micelles for glutathione-mediated intracellular drug delivery
Disulfide bridging strategies in viral and nonviral platforms for nucleic acid delivery
Single-component self-assembled RNAi nanoparticles functionalized with tumor-targeting iNGR delivering abundant siRNA for efficient glioma therapy
Dysregulation of glutathione synthesis in liver disease
Highly excretable gold supraclusters for translatable in vivo raman imaging of tumors
Nanoparticle–liver interactions: cellular uptake and hepatobiliary elimination
Sinusoidal efflux of glutathione in the perfused rat liver
Molecular probes for autofluorescence-free optical imaging
Molecular fluorescence and photoacoustic imaging in the second near-infrared optical window using organic contrast agents
In vivo near-infrared fluorescence imaging
rapid method to immunolabel large tissue samples for volume imaging
Intravenous delivery of siRNA targeting CD47 effectively inhibits melanoma tumor growth and lung metastasis
Gold nanoclusters-assisted delivery of NGF siRNA for effective treatment of pancreatic cancer
A phase I/Ib trial and biological correlate analysis of neoadjuvant SBRT with single-dose durvalumab in HPV-unrelated locally advanced HNSCC
Thiodigalactoside inhibits murine cancers by concurrently blocking effects of galectin-1 on immune dysregulation
angiogenesis and protection against oxidative stress
Cisplatin: a review of toxicities and therapeutic applications
Mannitol to prevent cisplatin-induced nephrotoxicity in patients with squamous cell cancer of the head and neck (SCCHN) receiving concurrent therapy
Survival and toxicity of weekly cisplatin chemoradiotherapy versus three-weekly cisplatin chemoradiotherapy for head and neck cancer: a systematic review and meta-analysis endorsed by the Italian Association of Radiotherapy and Clinical Oncology (AIRO)
Pembrolizumab in the first-line treatment of advanced head and neck cancer
Nivolumab for recurrent squamous-cell carcinoma of the head and neck
Pembrolizumab alone or with chemotherapy versus cetuximab with chemotherapy for recurrent or metastatic squamous cell carcinoma of the head and neck (KEYNOTE-048): a randomised
Cancer immunotherapy using checkpoint blockade
The evolving landscape of PD-1/PD-L1 pathway in head and neck cancer
Current studies of immunotherapy in head and neck cancer
Pembrolizumab versus cetuximab concurrent with radiotherapy in patients with locally advanced squamous cell carcinoma of head and neck unfit for cisplatin (GORTEC 2015-01 PembroRad): a multicenter
Tolerance and efficacy of pembrolizumab or cetuximab combined with RT in patients with locally advanced HNSCC (PembroRad). https://clinicaltrials.gov/study/NCT02707588
Study of pembrolizumab (MK-3475) or placebo with chemoradiation in participants with locally advanced head and neck squamous cell carcinoma (MK-3475-412/KEYNOTE-412). https://clinicaltrials.gov/study/NCT03040999
Immunogenic cell death in cancer and infectious disease
Radiation-induced bystander and abscopal effects: important lessons from preclinical models
Radiotherapy in combination with CD47 blockade elicits a macrophage-mediated abscopal effect
Using immunotherapy to boost the abscopal effect
Time to abandon single-site irradiation for inducing abscopal effects
Overcoming genetically based resistance mechanisms to PD-1 blockade
a first-in-class radioenhancer hafnium oxide nanoparticle
plus radiotherapy versus radiotherapy alone in patients with locally advanced soft-tissue sarcoma (Act.In.Sarc): a multicentre
Gold-nanocluster-mediated delivery of siRNA to intact plant cells for efficient gene knockdown
Influence of the size and charge of gold nanoclusters on complexation with siRNA: a molecular dynamics simulation study
Target-specific gene silencing of layer-by-layer assembled gold–cysteamine/siRNA/PEI/HA nanocomplex
Co-caged gold nanoclusters and methyl motifs lead to detoxification of dendrimers and allow cytosolic access for siRNA transfection
Radiotherapy remodels the tumor microenvironment for enhancing immunotherapeutic sensitivity
Tumor-reprogrammed resident T cells resist radiation to control tumors
The paradox of radiation and T cells in tumors
Fractionated radiation therapy stimulates antitumor immunity mediated by both resident and infiltrating polyclonal T-cell populations when combined with PD-1 blockade
Platinum-based chemotherapy plus cetuximab in head and neck cancer
Cetuximab for the treatment of colorectal cancer
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This study was supported by the following grants: P01CA257907 (to Q.T.L.
and J.L.) from the National Cancer Institute
and J.L.) from the National Institute of Dental and Craniofacial Research and U54CA274511 (to Q.T.L.) from the National Cancer Institute of the National Institutes of Health
Schematic illustrations were created using BioRender
The anti-galectin-1 blocking antibody (aGal-1) was generously provided by Bristol Myers Squibb via a material transfer agreement
Department of Pathology and Laboratory Medicine
Veterans Affairs Northern California Health Care System
developed supraclusters and performed in vitro characterization
shared P029 cell lines and laboratory resources
designed the in vivo clearance study and experiments on abscopal effect
are named inventors on a patent application related to the metabolizable supraclusters and their use in cancer treatments
The other authors declare no competing interests
Arta Monir Monjazeb and Jianping Xie for their contribution to the peer review of this work
(a) ROS production in MOC2 cells after incubation with PBS
or BSCgal (50 μg/mL) followed by RT (6 Gy)
ROS was indicated by green fluorescence from H2DCFDA probe
100 μm (b) Mean fluorescence intensity (MFI) of ROS production in MOC2 cells after various treatments (RT = 6 Gy; n = 5
GSC and BSCgal was determined by one-way ANOVA (P = 0.7288)
The others were analyzed by two-tailed unpaired Student’s t-test
not statistically significant; ns P (BSCgal + RT vs GSC + RT) = 0.7109; ****P < 0.0001
(c) Clonogenic survival assay of MOC2 cells various treatments (n = 3)
P value was determined by two-tailed unpaired Student’s t-test
(a) Quantification of CRT fluorescence intensity in Fig. 5b (n = 5)
(b) HMGB1 concentration in the plasma of mice after various treatments (n = 5)
(c) Box plot of percentage of GzmB+ cells in tumor-infiltrating CD8+ T cells from mice after various treatments (n = 5)
(d) Box plot of percentage of Ki67+CD8+ T cells in tumor- infiltrating CD45+ leukocytes from mice after various treatments (n = 5)
*P = 0.0319; **P (BSCgal vs GSC) = 0.0045; **P (BSCgal + SABR vs BSCgal) = 0.0082
GSC and BSCgal was determined by one-way ANOVA
The other P values were determined by two-tailed unpaired Student’s t-test
not statistically significant (P > 0.05)
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DOI: https://doi.org/10.1038/s41587-024-02448-0
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Efficient cytosolic delivery is a significant hurdle when using short interfering RNA (siRNA) in therapeutic applications
Here we show that cholesterol-rich exosomes are prone to entering cancer cells through membrane fusion
achieving direct cytosolic delivery of siRNA
Molecular dynamics simulations suggest that deformation and increased contact with the target cell membrane facilitate membrane fusion
In vitro we show that cholesterol-enriched milk-derived exosomes (MEs) achieve a significantly higher gene silencing effect of siRNA
inducing superior cancer cell apoptosis compared with the native and cholesterol-depleted MEs
as well as conventional transfection agents
When administered orally or intravenously to mice bearing orthotopic or subcutaneous tumours
the cholesterol-enriched MEs/siRNA exhibit antitumour activity superior to that of lipid nanoparticles
by modulating the cholesterol content of exosome membranes to facilitate cell entry via membrane fusion
we provide a promising approach for siRNA-based gene therapy
Thermostable ionizable lipid-like nanoparticle (iLAND) for RNAi treatment of hyperlipidemia
RNA silencing: from discovery and elucidation to application and perspectives
RNA interference-based therapy and its delivery systems
Rekindling RNAi therapy: materials design requirements for in vivo siRNA delivery
Oral delivery of nucleic acid therapeutics: challenges
Sphk2 RNAi nanoparticles suppress tumor growth via downregulating cancer cell derived exosomal microRNA
Tumour-derived extracellular vesicle membrane hybrid lipid nanovesicles enhance siRNA delivery by tumour-homing and intracellular freeway transportation
Targeted gene silencing in vivo by platelet membrane-coated metal-organic framework nanoparticles
Conformation-sensitive targeting of lipid nanoparticles for RNA therapeutics
Lysosome-related organelles as mediators of metal homeostasis
Targeted delivery of RNAi to cancer cells using RNA-ligand displaying exosome
A tumor targeted chimeric peptide for synergistic endosomal escape and therapy by dual-stage light manipulation
Visualizing lipid-formulated siRNA release from endosomes and target gene knockdown
Image-based analysis of lipid nanoparticle-mediated siRNA delivery
intracellular trafficking and endosomal escape
Design of synthetic materials for intracellular delivery of RNAs: from siRNA-mediated gene silencing to CRISPR/Cas gene editing
Nanoescapology: progress toward understanding the endosomal escape of polymeric nanoparticles
An antigen self-assembled and dendritic cell-targeted nanovaccine for enhanced immunity against cancer
Exosomes facilitate therapeutic targeting of oncogenic KRAS in pancreatic cancer
Extracellular vesicles as a next-generation drug delivery platform
Specificities of secretion and uptake of exosomes and other extracellular vesicles for cell-to-cell communication
Routes and mechanisms of extracellular vesicle uptake
Exosome uptake through clathrin-mediated endocytosis and macropinocytosis and mediating miR-21 delivery
Vesicle trafficking and vesicle fusion: mechanisms
and their implications for potential disease therapy
Enveloped viruses pseudotyped with mammalian myogenic cell fusogens target skeletal muscle for gene delivery
In situ cell membrane fusion for engineered tumor cells by worm-like nanocell mimics
A plant-derived natural photosynthetic system for improving cell anabolism
Membrane fusion and drug delivery with carbon nanotube porins
Folate-displaying exosome mediated cytosolic delivery of siRNA avoiding endosome trapping
SARS-CoV-2 requires cholesterol for viral entry and pathological syncytia formation
Different regions of synaptic vesicle membrane regulate VAMP2 conformation for the SNARE assembly
ABCA13 dysfunction associated with psychiatric disorders causes impaired cholesterol trafficking
Lipid raft microdomains and neurotransmitter signalling
Cholesterol reduction impairs exocytosis of synaptic vesicles
Minimal experimental requirements for definition of extracellular vesicles and their functions: a position statement from the International Society for Extracellular Vesicles
Mechanisms and kinetics of liposome-cell interactions
Temporal control of membrane fusion through photolabile PEGylation of liposome membranes
Exosomal lipid composition and the role of ether lipids and phosphoinositides in exosome biology
a coarse-grained force field for lipid membrane simulations with implicit solvent
Oral administration of bovine milk-derived extracellular vesicles induces senescence in the primary tumor but accelerates cancer metastasis
Methyl-beta-cyclodextrin induces mitochondrial cholesterol depletion and alters the mitochondrial structure and bioenergetics
Influence of cholesterol content on red cell membrane viscoelasticity and fluidity
Nanoscale imaging and mechanical analysis of Fc receptor-mediated macrophage phagocytosis against cancer cells
Hierarchical micro-/nanostructures from human hair for biomedical applications
Yolk-shell cationic liposomes overcome mucus and epithelial barriers for enhanced oral drug delivery
Efficient base editing in methylated regions with a human APOBEC3A-Cas9 fusion
Spatial transcriptomics at subspot resolution with BayesSpace
Programmably tiling rigidified DNA brick on gold nanoparticle as multi-functional shell for cancer-targeted delivery of siRNAs
Integrated combination treatment using a ‘smart’ chemotherapy and microRNA delivery system improves outcomes in an orthotopic colorectal cancer model
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We sincerely appreciate the financial support from the National Science Fund of Distinguished Young Scholars (82025032)
the National Key Research and Development Program of China (2022YFA1203200)
the National Natural Science Foundation of China (82073773)
the Young Elite Scientists Sponsorship Program by CAST (2022QNRC001)
the Key Research Program of Chinese Academy of Sciences (ZDBS-ZRKJZ-TLC005)
the ‘Open Competition to Select the Best Candidates’ Key Technology Program for Nucleic Acid Drugs of NCTIB (NCTIB2022HS01006)
Technology and Innovation (23HC1401200) and the Shanghai Institute of Materia Medica
Chinese Academy of Sciences (SIMM0220232001)
We thank the staff members of the Integrated Laser Microscopy System
the Molecular Imaging System and the Large-scale Protein Preparation System at the National Facility for Protein Science in Shanghai (NFPS)
The MD simulations were performed on BSCC-A6 at the Beijing Super Cloud Computing Center
These authors contributed equally: Yan Zhuo
State Key Laboratory of Drug Research and Center of Pharmaceutics
State Key Laboratory of Fluid Power and Mechatronic Systems
Shanghai University of Traditional Chinese Medicine
NMPA Key Laboratory or Quality Research and Evaluation of Pharmaceutical Excipients
National Institutes for Food and Drug Control
analysed the data and were involved in discussions of the data
All authors critically reviewed and approved the paper
Nature Nanotechnology thanks the anonymous reviewers for their contribution to the peer review of this work
3D distribution of 5%Chol/MEs in HCT116 cells
3D distribution of 30%Chol/MEs in HCT116 cells
Uncropped and unprocessed scans for Supplementary Fig
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DOI: https://doi.org/10.1038/s41565-024-01785-0
siRNAs are a new class of drugs with the potential to transform the way medicine is practiced
seven siRNA-based therapeutics have received regulatory approval
all targeting gene expression in the liver
specifically the ability to deliver to tissues outside the liver
have laid the foundation for the development of novel RNA-based therapeutics across a wide range of clinical indications
We collaborate with both academic and industry partners to accelerate the clinical translation of these compounds
Three of our drug candidates have now received regulatory approval to formally initiate clinical testing
with many more in various stages of preclinical development
Preeclampsia is a serious pregnancy complication characterized by high blood pressure and organ dysfunction
extrahepatic delivery platform to selectively knock down sFLT1
targeted approach to treating preeclampsia at its molecular origin
ALYS-101 – A lipophilic siRNA targeting JAK1
for the localized treatment of alopecia areata
Alopecia areata is an autoimmune disorder that causes patchy or total hair loss
ALYS-101 is a topically administered siRNA designed for local silencing of JAK1
enabling targeted immunomodulation without systemic side effects
RNA Therapeutics Institute
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upregulated midkine (MDK) limits the survival benefits conferred by temozolomide (TMZ)
RNA interference (RNAi) and CRISPR–Cas9 gene editing technology are attractive approaches for regulating MDK expression
delivering these biologics to GBM tissue is challenging
Here we demonstrate a polymer-locking fusogenic liposome (Plofsome) that can be transported across the blood–brain barrier (BBB) and deliver short interfering RNA or CRISPR–Cas9 ribonucleoprotein complexes into the cytoplasm of GBM cells
Plofsome is designed by integrating a ‘lock’ into the fusogenic liposome using a traceless reactive oxygen species (ROS)-cleavable linker so that fusion occurs only after crossing the BBB and entering the GBM tissue with high ROS levels
Our results showed that MDK suppression by Plofsomes significantly reduced TMZ resistance and inhibited GBM growth in orthotopic brain tumour models
Plofsomes are effective only at tumour sites and not in normal tissues
which improves the safety of combined RNAi and CRISPR–Cas9 therapeutics
Mechanisms of immunotherapy resistance: lessons from glioblastoma
Drug resistance in glioblastoma: a mini review
Dual functionalized brain-targeting nanoinhibitors restrain temozolomide-resistant glioma via attenuating EGFR and MET signaling pathways
Effects of radiotherapy with concomitant and adjuvant temozolomide versus radiotherapy alone on survival in glioblastoma in a randomised phase III study: 5-year analysis of the EORTC-NCIC trial
Interrogation of the microenvironmental landscape in brain tumors reveals disease-specific alterations of immune cells
DNA damage repair alterations modulate M2 polarization of microglia to remodel the tumor microenvironment via the p53-mediated MDK expression in glioma
DNA repair in personalized brain cancer therapy with temozolomide and nitrosoureas
Glioblastoma cell-derived lncRNA-containing exosomes induce microglia to produce complement C5
Nanoparticle-mediated convection-enhanced delivery of a DNA intercalator to gliomas circumvents temozolomide resistance
A biodegradable nanocapsule delivers a Cas9 ribonucleoprotein complex for in vivo genome editing
Single siRNA nanocapsules for effective siRNA brain delivery and glioblastoma treatment
Multistage delivery nanoparticle facilitates efficient CRISPR/dCas9 activation and tumor growth suppression in vivo
NanoRNP overcomes tumor heterogeneity in cancer treatment
Precise targeting of POLR2A as a therapeutic strategy for human triple negative breast cancer
Image-based analysis of lipid nanoparticle–mediated siRNA delivery
Rational design of cancer nanomedicine: nanoproperty integration and synchronization
Integration of nanoassembly functions for an effective delivery cascade for cancer drugs
Nanomechanical action opens endo-lysosomal compartments
maintenance and disruption of the blood-brain barrier
Neuroprotective nanoscavenger induces coaggregation of β-amyloid and facilitates its clearance in Alzheimer’s disease brain
Self-immolative hydroxybenzylamine linkers for traceless protein modification
Acid-labile traceless click linker for protein transduction
Site-specific chemical modification of antibody fragments using traceless cleavable linkers
Reactive oxygen species‐responsive protein modification and its intracellular delivery for targeted cancer therapy
Dual‐locking nanoparticles disrupt the PD‐1/PD‐L1 pathway for efficient cancer immunotherapy
Protein toxin chaperoned by LRP‐1‐targeted virus‐mimicking vesicles induces high‐efficiency glioblastoma therapy in vivo
and avoiding the endosome: peptide‐targeted
fusogenic porous silicon nanoparticles for delivery of siRNA
Fusogenic liposomes encapsulating mitochondria as a promising delivery system for osteoarthritis therapy
Tumor cell surface modification with immuno-amplified nanoparticles to enhance cancer immunotherapy
Fusogenic liposomes as nanocarriers for the delivery of intracellular proteins
Strategies for the intracellular delivery of nanoparticles
Membrane‐fusion‐mediated multiplex engineering of tumor cell surface glycans for enhanced NK cell therapy
Monensin enhanced generation of extracellular vesicles as transfersomes for promoting tumor penetration of pyropheophorbide-a from fusogenic liposome
Targeted fusogenic liposomes for effective tumor delivery and penetration of lipophilic cargoes
Anti-phagocytosis-blocking repolarization-resistant membrane-fusogenic liposome (ARMFUL) for adoptive cell immunotherapy
A multistage cooperative nanoplatform enables intracellular co‐delivery of proteins and chemotherapeutics for cancer therapy
In situ modification of the tumor cell surface with immunomodulating nanoparticles for effective suppression of tumor growth in mice
Bi-specific macrophage nano-engager for cancer immunotherapy
Microenvironment remodeling micelles for Alzheimer’s disease therapy by early modulation of activated microglia
Biocompatible polymeric nanoparticles degrade and release cargo in response to biologically relevant levels of hydrogen peroxide
Fluorescamine: a reagent for assay of amino acids
Stapled liposomes enhance cross‐priming of radio‐immunotherapy
Polymer‐reinforced liposomes amplify immunogenic cell death‐associated antitumor immunity for photodynamic‐immunotherapy
Measurement of co‐localization of objects in dual‐colour confocal images
Detection of DNA double-strand breaks by gamma-H2AX immunodetection
Delivery of CRISPR-Cas tools for in vivo genome editing therapy: trends and challenges
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This study was supported by the (1) National Natural Science Foundation of China (numbers 82372901 and 82073298 for J.C.
(2) Heilongjiang Provincial Key R&D Project (number GA21C002 for J.C
(3) Heilongjiang Provincial Key Project of The Educational Science 14th Five-Year Plan (number GJB1422780 for J.C.)
(4) Heilongjiang Provincial Natural Science Foundation (number LH2022H022 for X.M.)
(5) China Postdoctoral Science Foundation (numbers 2019M660074 and 2022T150173 for X.M.)
(6) Heilongjiang Postdoctoral Science Foundation (numbers LBH-Z19029 and LBH-TZ2218 for X.M.) and (7) Harbin Medical University Marshal Initiative Funding (number HMUMIF-22009 for X.M.)
These authors contributed equally: Yu Zhao
The Second Affiliated Hospital of Harbin Medical University
The Sixth Affiliated Hospital of Harbin Medical University
Key Laboratory of Functional Polymer Materials of Ministry of Education
State Key Laboratory of Medicinal Chemical Biology
All authors discussed the results and commented on the paper
Nature Nanotechnology thanks Pablo del Pino and the other
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DOI: https://doi.org/10.1038/s41565-024-01769-0
when things turn out the opposite of what you expect
it's often the starting point for discovery
That's what happened to a team of researchers from Memorial Sloan Kettering Cancer Center (MSK) and their collaborators at the Icahn School of Medicine at Mount Sinai
Their unexpected findings in the lab point to an opportunity to improve therapies that use small RNAs to silence disease-causing genes
potentially including those involved in cancer
but when it doesn't turn out the way you planned
it can lead you to find something else that's much more interesting."
the researchers - led by Seungjae Lee
a postdoctoral fellow in the Lai Lab at MSK's Sloan Kettering Institute - were testing how a protein called ALAS1 helps to make small regulatory RNAs called microRNAs
they expected to see levels of microRNAs drop
we were surprised to see them increase," Dr
That counterintuitive result led to the discovery of an unrecognized role for ALAS1 beyond its well-known role in the production of heme
(Heme is an important player in many biological processes
including in oxygen transport - giving hemoglobin its name - in energy production
The team's findings were published in Science
one of the world's most prestigious scientific journals
Both microRNAs and the related class of small interfering RNAs (siRNAs) are small snippets of RNA - just 21 or 22 nucleotides long - that bind to specific messenger RNAs (mRNAs) and repress them
There's a bucket brigade of players that together convert longer RNA molecules into the tiny active products
and a key takeaway is that scientists have harnessed this knowledge to turn small RNAs into drugs that can silence genes that cause specific diseases
Food and Drug Administration (FDA) in 2018 to treat a debilitating genetic disorder called hereditary transthyretin amyloidosis
A handful of additional siRNA drugs have been approved since
with more moving their way through clinical trials
Doctors see great potential to develop siRNA medicines against both rare diseases and more common ones (siRNA drugs are sometimes called RNAi drugs
meaning they work by interfering with messenger RNA accumulation)
Lee had discovered that upon removing ALAS1 from cells
And further experiments showed that removing any of the other enzymes in the heme biosynthesis pathway did not affect microRNA levels
"This told us that ALAS1 has another job outside of helping to make heme
"We can consider this a 'moonlighting' function," Dr
"And here we discovered that ALAS1 has this secret role regulating microRNAs that's not connected to its normal role in heme synthesis."
The discovery led the MSK researchers to partner with colleagues from the Icahn School of Medicine at Mount Sinai who specialize in heme regulation and ALAS genes - Makiko Yasuda
This allowed the MSK researchers to extend their findings from cell culture into custom animal models that the Mount Sinai group were developing
removing ALAS (specifically in liver cells) led to a global increase in microRNAs
"The emerging picture is that ALAS acts as a brake on the production of microRNAs," Dr. Lai says. "So we thought, now that we know how to remove this brake, maybe we can use that to improve the efficacy of siRNA drugs and their ability to silence their target genes."
this knowledge might help boost the activity of siRNA drugs against any problematic gene that is overactive in disease
Potentially this could include oncogenes known to drive cancer
"But we're not quite there yet," he says
"Therapeutic siRNA drugs don't work well enough against all targets and are currently limited in where they can be used in the body." In fact
all six of the FDA-approved siRNA drugs target hepatocytes in the liver
"It's straightforward to get drugs into the liver
which serves as a filter for the body," Dr
the team showed that not only could they deplete mouse liver cells of ALAS
but doing so also enhanced the silencing activity of another model siRNA compound delivered to the mice
one of the six approved siRNA drugs turns off ALAS1 to treat acute hepatic porphyrias
Desnick worked on the preclinical and clinical trials for the drug
Since an siRNA against ALAS1 works effectively and safely in humans
this raises the possibility of combining such an agent to enhance other siRNA drugs
Lai notes that this strategy could be generally applicable to any siRNA
And if siRNA drugs can be made to work better
this could improve their cost-effectiveness
reduce side effects by making them effective at lower doses
and perhaps help to target additional cell types beyond liver cells
was awarded the Nobel Prize with Victor Ambros
for their joint discovery of microRNA and its role in gene regulation in the early 1990s
Lai did his undergraduate thesis research in Dr
Ruvkun's lab at that time (on another class of gene regulator) and credits him for launching his own career
"I got my first real exposure to how science was actually done and gained lifelong interests in developmental biology and small RNAs," Dr
adding that his mentor's recent accolade underscores the importance of curiosity-driven research
Ruvkun didn't start out looking for microRNAs," Dr
he was investigating the development of nematodes
And not only did this unveil an entirely new paradigm for how genes are controlled
the field they started eventually resulted in a novel class of human therapies
"When people ask why we're not spending all of our research dollars directly studying diseases like cancer
why we're funding research into cells and processes in model organisms like fruit flies
and bacteria - this is a great example of how discovery science fuels the biggest breakthroughs," he continues
"And I think it is especially critical to keep this conversation active
given how much uncertainty and disagreement there is in society and government about how much to publicly fund scientific research and in what areas
there will be continued support to keep the engine of foundational research strong."
Funding for the research includes grants from the National Institutes of Health (R01DK134783
P30-CA008748); a Cooperative Centers of Excellence in Hematology pilot grant (10040500-05S1); and a NYSTEM training award (C32559GG)
The researchers have filed a patent application on their methods for enhancing the efficacy of RNAi therapy by targeting ALAS1/ALAS2 (WO2024148236A1)
Yasuda and Desnick are also co-inventors of a patent for RNAi therapy of acute hepatic porphyrias
They also report pharmaceutical consulting work
Memorial Sloan Kettering Cancer Center
Lee, S., et al. (2024). Noncanonical role of ALAS1 as a heme-independent inhibitor of small RNA–mediated silencing. Science. doi.org/10.1126/science.adp9388
Posted in: Medical Science News | Medical Research News
A biochemical breakthrough using simple carbon atoms by Ken Yamada, PhD, and Anastasia Khvorova, PhD, has dramatically improved the stability and efficacy of a potential oligonucleotide therapeutic platform in mice. This discovery, published in Nature Biotechnology
has the potential to improve the durability of oligonucleotide drugs
and to bring these therapies to cell types outside of the liver for the first time
“The innovation of our study is a modification to the chemical composition behind the oligonucleotide platform’s architecture,” said Dr
the Remondi Family Chair in Biomedical Research and professor of RNA therapeutics
“Using a relatively simple change—extending the RNA backbone with single carbon atoms—we’ve been able to significantly improve the duration that oligonucleotides persist in cells by effectively hiding them from the nucleases that normally break them up
This type of modification is critical to the success of oligonucleotide drugs as a class.”
are a new class of medicine that enables modulation of disease-causing genes for therapeutic effect
There are six siRNAs approved for clinical use by the Food and Drug Administration—all in the liver—with more in late-stage clinical trials
was approved in 2018 for people with hereditary transthyretin-mediated amyloidosis
The enzymes responsible for breaking down oligonucleotide molecules
giving the drugs a limited amount of time to achieve a therapeutic effect
scientists have been challenged to design chemical scaffolds that can stabilize
sustain and extend the longevity of oligonucleotide drugs necessary to achieve therapeutic success in living tissue
Most oligonucleotide modifications focus on changing the phosphorothioates or sugar molecules existing in the chemical backbone
homing in on the carbon molecules in the backbone’s chemical structure
a single or a few methylations to nucleobases and amino acids have been shown to slightly alter the structure of DNA
RNA and proteins that profoundly impacts in-cell gene expression
small structural change making a big impact in the cell,” said Yamada
“This process inspired us to apply an analogous approach to the oligonucleotide platform’s backbone—a small structural change making a big impact on siRNA’s durability by increased stability and enhanced efficacy”
“If we could garner even a 10-fold increase in persistence we could reduce dosage or clinical treatment time from once every two weeks to every five months
To have a 32-fold increase in mice models is tremendously encouraging.”
Yamada and Khvorova found that an extra carbon atom inserted in the correct spot along the nucleoside effectively hid the oligonucleotide molecules from degradation by the nuclease enzyme
This resulted in a more stable and efficient oligonucleotide
which was dubbed extended nucleic acid or exNA
that persisted 32-fold longer than its phosphorothioate-modified counterparts
“It’s all about where and how you add the carbon,” said Yamada
“Even a slight structural modulation can have a huge impact on efficacy if you do it in the right place and in the right way.”
eye—a host of tissues and diseases that were beyond our capabilities are now potentially feasible drug targets for oligonucleotide therapies.”
The next step for researchers going forward is to begin testing the safety and longevity of their oligonucleotide backbone in clinical trials
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Small interfering RNAs (siRNA) technology has emerged as a promising therapeutic tool for human health conditions like cancer due to its ability to regulate gene silencing
their delivery remains localized and limiting their systemic use
This study used single-walled carbon nanotubes (SWNTs) functionalized with polyethylene glycolated (PEGylated) phospholipids (PL-PEG) derivatives for systemic siRNA delivery
We developed an siRNA systemic delivery vehicle (SWNT-siRNA) by conjugating SWNT functionalized with PL-PEG containing either amine (PA) or maleimide (MA)
The functionalized SWNT with a lower molecular weight of PA produced the SWNT-siRNA conjugate system with the highest stability and high siRNA loading quantity
The system delivered siRNA to a panel of tumour cell lines of different organs (i.e
H1299 and MCF-7) and a non-cancerous human embryonic kidney 293 cells (HEK293T) with high biocompatibility and low toxicity
The cellular uptake of SWNT-siRNA conjugates by epithelial cells was found to be energy dependent
did not inhibit SWNT-mediated siRNA delivery
Mouse xenograft model further confirmed the potential of SWNT-siRNA conjugates with a significant gene knock-down without signs of acute toxicity
These findings pave the way for potential gene therapy applications using SWNTs as delivery vehicles
While these agents showed promising results
their application is primarily limited to localized delivery to a certain target organ
This limitation makes these agents less useful for systemic diseases such as cancers that can metastasise to other organs
or genetic diseases that affect multiple organ systems
it is pivotal to break through this challenge to design an effective siRNA agent for the treatment of systemic diseases
Our team has successfully optimised the functionalization of SWNTs using different molecular weights of the PL-PEG reactive group (PA or MA)
followed by a series of investigation of the efficiency of siRNA loading on these SWNT-PL-PEGylated carriers
including their knock-down efficiency and the toxicity of the SWNT-siRNA conjugates on various cancer cell lines along with its cellular uptake mechanisms
We also demonstrated the efficient gene knock-down in mouse xenograft model verifying the success of this siRNA system for systemic gene delivery
Our work demonstrates the potential of the SWNT-PL-PEGylated vehicle as a promising delivery system of siRNA in gene therapy applications
Schematic drawing processing flow of functionalization of single-walled carbon nanotubes (SWNT) with PL-PEG-NH2 and PL-PEG-maleimide
(C) Aqueous suspensions of SWNT (pristine)
SWNT-PL-PEG-S-S-siRNA and SWNT-PL-PEG-siRNA
(Picture taken by authors with a Canon EOS 5 Fujichrome Velvia)
Table 1 summarises the yield of functionalized SWNT and their subsequent conjugation with siRNA
Despite a relatively low yield of functionalized SWNT from this process
these functionalized SWNT were able to be conjugated with 5’-thiolated siRNA to produce SWNT-PL-PEG-S-S-siRNA and SWNT-PL-PEG-siRNA
It was found that the siRNA loading capacity into these functionalized SWNT ranged from 35 to 44% for the PA functional group and 29–45% for MA functional group; with a decrease in siRNA loading capacity as the molecular size of the PEG functional group increased
zeta potential measurements revealed that the SWNT-siRNA conjugates were stable in aqueous solutions with values of -38.24 ± 5.28 mV for SWNT-PL-PEG-S-S-siRNA and − 32.78 ± 3.76 mV for SWNT-PL-PEG-siRNA
Particle size analyses showed average sizes of 617 ± 115 nm and 703 ± 210 nm for the respective SWNT-siRNA conjugates
slightly larger than the functionalized SWNT but within the appropriate range for cellular infiltration
which is a critical factor for a successful transfection
These findings demonstrate an efficient loading of siRNA using functionalized SWNT
Significant gene silencing efficiency using SWNT-siRNA conjugates
(A) Graphical representation of SWNT-PL-PEG-S-S-siRNA
(B) Graphical representation of SWNT-PL-PEG-siRNA
D and E) Evaluation of gene silencing effect by SWNT-PL-PEG-S-S-siGFP and SWNT-PL-PEG-siGFP conjugates in MCF-7
Cells expressing stable green fluorescent protein (GFP) were treated with SWNT-PL-PEG-S-S-siGFP or SWNT-PL-PEG-siGFP conjugates at a concentration of 100 nM siGFP
The cell nuclei were stained with DAPI (blue)
Microscopic observation was captured under 100x magnification
Bars represent mean ± SD of at least 3 independent experiments
* represents statistical significance as compared to vehicle controls (Student’s t-test
To ensure that the observed reduction of GFP signals was not due to the toxic effects of SWNT-PL-PEG-S-S-siGFP or SWNT-PL-PEG-siGFP conjugates, the cytotoxic effects of SWNT-PL-PEG-S-S-siGFP or SWNT-PL-PEG-siGFP conjugates on these cell lines were determined using the LDH release assay at 72 h after treatment. As shown in Supplement Figure S1
neither the SWNT-PL-PEG-S-S-siGFP nor SWNT-PL-PEG-siGFP conjugates significantly affected cell viability
implying the non-toxic nature of SWNT-siRNA conjugates
Dual-silencing efficacy of siRNA-conjugated SWNT delivery system
Fluorescence microscopic images of co-expressed GFP and RFP in H1299 cells incubated with 100 nM of (A) SWNT-PL-PEG-S-S-siRNA or (B) SWNT-PL-PEG-siRNA conjugates targeting GFP (siGFP) or RFP (siRFP) or LUC (siLUC; negative control) alone
or both (dual targeting; siGFP + siRFP) for 72 h
The furthest right panel was the combined images
Energy dependent cellular internalization mechanisms of SWNT-siRNA conjugates independent of ABCB1
Graph shows the mean relative luminescent units (RLU) of (A and B) luciferase expressing H1299 cells co-treated with SWNT only (without siLUC)
SWNT-PL-PEG-S-S-siLUC or SWNT-PL-PEG-siLUC with or without sub-lethal concentrations of various endocytosis inhibitors
genistein and m-βCD are inhibitors for energy-dependent cellular uptake
caveolae-dependent endocytosis and macro-pinocytosis
* represents statistical significance as compared to SWNT-siLUC (Student’s t-test
(C) Western blot of ABCB1 and loading control GAPDH
Ectopic expression of ABCB1 (multiple drug resistance) protein in H1299-LUC cells was confirmed by the immunoblotting with increased expression of ABCB1 at 141 kDA
while GAPDH at 36 kDA served as the loading control
Full blots available in Supplementary Figure S2-S3
(D) Expression of ABCB1 did not affect the delivery of siRNA by the SWNT
* represents statistical significance as compared to controls (Student’s t-test
The findings suggest that the cellular uptake of SWNT-siRNA is not impacted by ABCB1-mediated efflux
indicating that SWNTs could potentially serve as effective carriers for gene therapy in multiple drug-resistant tumours
Significant knock-down efficacy using SWNT-PL-PEG-S-S-siRNA conjugate in mouse xenograft model
(A) In vivo bioluminescence imaging of luciferase expressing HCT-116 xenograft in BALB/C nude mice
The images show intensity of luminescence as ‘heat’ maps in which red is the maximum intensity
The scale shows the number of photons detected
(Left) Mice were treated with saline PBS as negative controls while (right) mice were injected with single dose of SWNT-PL-PEG-S-S-siLUC at 0.8 mg/kg through tail-vein
(B) Significant gene knock-down by SWNT-PL-PEG-S-S-siLUC in mouse xenograft model
Quantitation of bioluminescence was determined as depicted in Methods
* indicates statistical significance as compared to vehicle control (Student’s t-test
(C) No significant body weight loss was observed following administration of SWNT-PL-PEG-S-S-siLUC to the HCT-116 xenograft in BALB/C nude mice
While the promise of CNTs as nanocarriers is undeniable
rigorous research and optimization are required to overcome these limitations
PL-PEG functionalization aligns the physicochemical properties of SWNTs with the requirements of an effective systemic delivery system
ensuring that the therapeutic potential of siRNA is fully utilized
Our findings demonstrated a low yield of SWNT functionalization
this maybe due to the dispersion of SWNT which can be improved further by optimizing sonication parameters
and mildly oxidizing of the SWNT in the future studies
we could further explore improving the recovery by redispersing the functionalized SWNT in a suitable solvent if necessary
minimizing losses during purification and handling
Future mechanistic studies using fluorescent or radiolabelled tracking as well as targeted cleavage mechanisms
as compared with the commercial siRNA delivery kit
the uptake of SWNT-PL-PEG-S-S-siRNA and SWNT-PL-PEG-siRNA was not affected by the presence of P-glycoprotein
a membrane protein often associated with drug resistance
This observation suggests that SWNTs could be applied in delivering agents that could be beneficial in treating drug-resistant tumours
addressing a significant challenge in cancer treatment
it is certainly warranted to investigate whether co-delivery with other synthetic compound or biological molecule may further improve its efficacy
the research findings highlight the promising potential of SWNT-siRNA conjugates as gene-silencing tools
Their capability to silence multiple genes simultaneously
and their effectiveness in drug-resistant conditions are promising aspects for cancer treatment
The transition from in vitro to in vivo efficiency is a crucial step in drug development
and the success of SWNT-siRNA conjugates in animal models provides a promising lead for future investigations
Cylindrical structure SWNT were functionalized as previously described66
1 mg HiPCo® SWNT with a diameter of approximately 1.0 nm (ranging between 0.8 nm and 1.2 nm) and individual SWNT length between 100 nm and 1000 nm
with high aspect ratio (length to radius) is typically ranging between 8,333 and 12,500; and > 95% purity (Unidym Inc.
either PL-PEG-NH2 (PA) or PL-PEG-maleimide (MA) (NOF America Corporation
were dissolved in 5 mL diethylpyrocarbonate (DEPC)-treated water (nuclease-free)
This mixture was sonicated for 60 min in a water bath at room temperature (approximately 22 °C)
PEG derivatives and PEG chains of varying molecular weights (2000
Insoluble contaminants and bundled SWNT were eliminated through centrifugation using a Beckman Coulter Optima L-90 K Ultracentrifuge (Beckman Coulter
USA) at 24,000 × g for 6 h at room temperature
the supernatant was collected and further centrifuged for 10 min at 4,000 × g at room temperature using an Amicon centrifugal filter with a cut-off size of 100 kDa (Millipore
The residues underwent five rounds of washing using water to ensure a thorough removal of excess PL-PEG from the SWNT solution
the SWNT concentration was determined using an ultraviolet-visible spectrometer (Perkin Elmer
Both the SWNT-PL-PEG-S-S-siRNA and SWNT-PL-PEG-siRNA conjugates were prepared as described above
and transferred into plastic optical cuvettes
Dynamic light scattering (DLS) and zeta potential measurements were performed using Malvern Zen Zetasizer Nano (Malvern Instrument
Hydrodynamic dimensions of SWNT in suspension were determined by automatic software analysis of dynamic light scattering autocorrelation curves
Zeta potentials were measured in Malvern Instruments Folded Capillary Cells with embedded electrodes
Each measurement consisted of up to 100 runs from which the average zeta potential value was calculated
human non-small cell lung carcinoma line H1299
and human cervical cancer cells HeLa were procured from the American Type Culture Collection (ATCC; Manassas
They were cultured in RPMI 1640 medium (Sigma-Aldrich
USA) fortified with 10% fetal bovine serum (FBS
Singapore) and 1% penicillin-streptomycin (Biowest
American Type Culture Collection) was maintained in Dulbecco’s Modified Eagle’s Medium (DMEM; Sigma-Aldrich
USA) enriched with 10% fetal bovine serum and 1% penicillin-streptomycin
All cell lines were kept in logarithmic growth inside a 37 °C humidified incubator with an atmosphere of 5% CO2
Stable expressions of green fluorescent protein (GFP)
luciferase mRNA (LUC) and ABCB1 were established in MCF-7
HEK-293T and HeLa using lentiviral transduction
Lentiviral expression plasmids were purchased from OriGene (Rockville
Lentiviral stocks were produced by co-transfection with 5 µg of packaging plasmids psPAX2 (Addgene; plasmid 12260) and 5 µg envelope plasmids pMD2.G (Addgene; plasmid 12259) into HEK-293T cells as described previously using CalPhosTM Mammalian Transfection Kit (Clontech
and/or LUC were seeded overnight at a density of 3 × 105 cells per 60 mm culture dish
or 5 × 103 cells per well on a 96-well culture plate
100 nM of siRNA conjugated to SWNT-PL-PEG-S-S-siRNA or SWNT-PL-PEG-siRNA was introduced to the cells expressing GFP
The siRNA concentration was calculated based on an absorbance at 260 nm
and/or LUC post-transfection were assessed at 72 h using the Eclipse Ti-U inverted fluorescent microscope (Nikon
Quantitative measurements were conducted using the Infinite F200 microplate reader (Tecan Group
Statistical significance was assessed using Student’s t-tests
Values of P < 0.01 were considered statistically significant (*)
All data are presented as mean ± standard deviation (SD)
Cell viability assay was performed using CellTiter-Glo® Luminescent Cell Viability Assay (Promega
USA) as according to manufacturer’s protocol and previous studies [24,26]
Quantitative measurements were conducted using a SpectraMax Plus 384 Microplate Reader (Molecular Devices
To determine the cellular update efficiency
H1299 cells expressing luciferase (H1299-LUC) were pre-treated with sublethal concentration of sodium azide
or methyl-b-cyclodextrin (m-βCD; 5 mM) 30 min prior to incubation with SWNT-siLUC conjugates
NaN3 may inhibit energy-dependent cellular uptake [27]
while chlorpromazine may block clathrin-mediated endocytosis [28]
Genistein and m-βCD may inhibit caveolae-dependent endocytosis and macro-pinocytosis
The inhibitory effects of each pathway were verified by assessing the silencing efficiency of firefly luciferase expression by the SWNT-PL-PEG-S-S-siLUC or SWNT-PL-PEG-siLUC conjugates after 72 h incubation
Luciferase expression and cell viability were measured using the ONE-Glo™ + Tox Luciferase Reporter and Cell Viability Assay (Promega
Luminescence signals were read using the SpectraMax Plus 384 Microplate Reader (Molecular Devices
USA) and normalised against signals from untreated cells
Primary and secondary antibodies targeting ABCB1 and GAPDH (as the loading control) were sourced from Santa Cruz Biotechnology
The results were viewed using ChemiDoc™ XRS + molecular imager (Bio-Rad Laboratories
in vivo bioluminescence assessments were carried out daily for a week
Tumour dimensions were logged bi-weekly using a calliper
and volumes were calculated as: V = 0.5 a × b2 (where ‘a’ and ‘b’ represent the tumour’s long and short diameters
mice were given 150 mg/kg luciferin intraperitoneally
the mice were anesthetised using the mixture of oxygen and isoflurane
they were placed in an imaging chamber for bioluminescence measurements using IVIS® Lumina II optical imaging system (Caliper Life Sciences
Bioluminescence images from the whole body
inclusive of primary and metastatic tumours
The primary study endpoint was tumour growth rate
(n = 5) and statistically significant differences were concluded using independent t-test when p value less than 0.05
All data generated or analysed during this study are included in this published article (and its Supplementary Information files)
FDA approves patisiran to treat hereditary transthyretin amyloidosis
Ongoing clinical trials of nonviral siRNA therapeutics
Clinical advances of siRNA-based nanotherapeutics for cancer treatment
siRNA could be a potential therapy for COVID-19
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Overcoming barriers for siRNA therapeutics: from bench to bedside
Functionalized single-walled carbon nanotubes: cellular uptake
biodistribution and applications in drug delivery
Nucleic acid drug and delivery techniques for disease therapy: Present situation and future prospect
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with particular emphasis on potential applications in biomedicine
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Functionalized carbon nanotubes: synthesis
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Carbon nanotubes as an emerging nanocarrier for the delivery of doxorubicin for improved chemotherapy
Synthetic strategies in construction of organic macromolecular carrier-drug conjugates
Modeling prostate cancer: what does it take to build an ideal tumor model
A nanoprimer to improve the systemic delivery of siRNA and mRNA
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This research was funded by Ministry of Higher Education
the Hubert Curien Partnership – Hibiscus (PHC-HIBISCUS) France-Malaysia (Grant no
Technology and Innovation Nanotechnology Research Grant (NND/NA/1/TD11-002) and UCSI University Research Excellence and Innovation Grant (REIG-FPS-2023/038)
Kandiah Faculty of Medicine and Health Sciences
Center for Nanotechnology and Advanced Materials
analyzed the results and wrote the first draft of the manuscript
provided intellectual input and troubleshooting
secured fundings and revised the manuscript
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DOI: https://doi.org/10.1038/s41598-024-80646-1
Phase 2 trial of zerlasiran yields first demonstration of longer effect with each dose of an siRNA
reduced time-averaged Lp(a) concentrations by more than 80% across 36 weeks of treatment in the randomized ALPACAR-360 trial
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“We are still learning how the siRNA therapies affect lipoprotein(a) during extended treatment
This trial shows for the first time that with each successive dose
Lp(a) reduction endured longer and waned more slowly
This has implications for the design of phase 3 trials of zerlasiran and potentially for optimal dosing of other drugs in this class.”
Zerlasiran is among several medications in clinical trials for reduction of elevated Lp(a)
a genetically determined risk factor for atherosclerotic cardiovascular disease (ASCVD) that is resistant to traditional preventive therapies
No pharmacotherapies have been approved for Lp(a) reduction
The investigational therapies furthest in development are four nucleic acid therapeutics
consisting of the antisense oligonucleotide pelacarsen and three siRNAs
“Identifying the best dosing strategy for siRNA therapies is difficult because they all have prolonged durations of action that range from weeks to months,” says Dr
Chief Academic Officer of Cleveland Clinic’s Heart
who is involved with clinical trials of three of the four nucleic acid therapeutics
“Along with assessing the safety of zerlasiran
ALPACAR-360 was designed to help identify the best dose and dosing frequency to guide a phase 3 trial.”
The study involved 180 adults with stable ASCVD from 26 sites in Europe
All patients had a serum Lp(a) concentration of at least 125 nmol/L
a threshold that confers increased cardiovascular risk
with a mean age of 63.7 years and a median baseline Lp(a) of 213 nmol/L (interquartile range
Patients were randomized in a double-blind manner to one of five treatment groups:
Doses were injected subcutaneously in the abdomen
Patients were followed every four weeks up to 40 weeks and then at weeks 48 and 60 after randomization
The primary endpoint was the time-averaged percentage change in serum Lp(a) from baseline through 36 weeks after first administration
Time-averaged percentage changes from baseline to weeks 48 and 60 were secondary endpoints
as were safety and tolerability through 60 weeks
The Cleveland Clinic Coordinating Center for Clinical Research (C5Research) performed statistical analysis and helped manage the trial
178 received study doses and were included in results analyses
mean time-averaged percentage changes in Lp(a) concentrations through 36 weeks were:
Median percentage changes at week 36 were:
Injection-site reactions were the most common treatment-related adverse effects; mild pain at the site was reported by 2.3% to 7.1% of participants within the first day after injection
No such reactions led to study withdrawal or missed doses
and no treatment-related serious adverse events occurred
“This is the first trial of a nucleic acid therapy to use time-averaged Lp(a) reduction as an endpoint,” Dr
noting that other trials used maximal reduction or reduction at a given time point
“Our endpoint more accurately reflects the effect of treatment over time
the duration of reduction was longer and the waning of Lp(a) lowering was attenuated,” he continues
“In the group that received three doses of zerlasiran 300 mg
the median reduction at the 60-week final follow-up visit was still 58.8%
This was a full 28 weeks after the last of the three doses had been given.”
He adds that any such effect hadn’t been appreciated in previous trials of nucleic acid therapies because they have involved either single doses or agents that are dosed too frequently — such as every 4 or 12 weeks — to adequately gauge the effect on Lp(a) rebound
“The cumulative effect we observed with successive doses will inform the dosing interval chosen for phase 3 studies of zerlasiran,” Dr
the study report includes waterfall plots that reveal responses to therapy on a patient-by-patient basis
The plot for patients who received a dose every 16 weeks showed consistent responses to therapy with zerlasiran 300 mg
suggesting that dosing every 16 weeks may provide more uniformly substantial reduction across all patients compared with dosing every 24 weeks
“The question that naturally arises is how much Lp(a) reduction is enough,” Dr
That answer is awaiting results from ongoing outcomes-based phase 3 trials of three agents — pelacarsen and the siRNAs olpasiran and lepodisiran
“The collective research community is taking a lot of shots on goal to finally address the morbidity and mortality from Lp(a) elevation,” Dr
“We are hopeful at least one of them will end up in the back of the net soon.”
“It is exciting to have so many drugs in development to lower Lp(a),” adds Leslie Cho, MD
Co-Section Head of Preventive Cardiology and Rehabilitation at Cleveland Clinic
“We look forward to results from phase 3 studies to tell us whether lowering Lp(a) in the era of aggressive LDL control reduces cardiac events.”
The trial was funded by Silence Therapeutics
Nissen reported coordinating center funding from Silence Therapeutics
Novartis and Eli Lilly during the conduct of the trial
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Hybrid seed failure arising from wide crosses between plant species is a recurring obstacle in plant breeding
This postzygotic reproductive barrier primarily occurs in the endosperm
a tissue that nourishes the embryo and functions similarly to the placenta in mammals
We found that incompatible seeds show a loss of DNA methylation and chromatin condensation in the endosperm
similar to seeds lacking maternal RNA polymerase IV activity
This similarity is linked to a decrease in small interfering RNAs in the endosperm (sirenRNAs)
maternal RNA polymerase IV-dependent short interfering RNAs that regulate DNA methylation
Several AGAMOUS-like MADS-box transcription factor genes (AGLs)
are targeted by sirenRNAs in cis and in trans
This finding aligns with the enrichment of AGL target genes among deregulated genes
We propose that hybrid seed failure results from reduced maternal sirenRNAs combined with increased AGL expression
leading to abnormal gene regulation in the endosperm
implying the existence of a dosage-sensitive element contributing to this reproductive barrier within the endosperm
the precise nature of this component remains elusive
whether sirenRNAs constitute the dosage-sensitive component determining hybridization success remains an open question
we demonstrate that the loss of maternal Pol IV function mirrors the loss of chromatin condensation and DNA methylation observed in Capsella hybrids
This resemblance in phenotype is correlated with a shared decrease in sirenRNAs
which regulate target genes in cis and trans by guiding DNA methylation
Among these sirenRNA targets are several AGLs
aligning with the enrichment of AGL target genes among deregulated genes
we propose that the response to interspecies and interploidy hybridizations is instigated by two factors: the depletion of maternally derived sirenRNAs and the heightened expression of AGLs targeting hypomethylated regions in hybrid endosperm
Cleared hybrid Capsella seeds at 4 to 6 DAP
The corresponding mature seeds are shown on the right side of each panel
100 µm and 1 mm for cleared and mature seeds
The colour code reflects effective ploidy as indicated in the figure
Mature seed phenotypes of crosses Cr × Cbp and Cbp × Cr
Mature seed phenotypes of crosses Co × Cr and 4xCo × Cr
Germination data for the crosses shown in c
Shown is the fraction of germinating seeds from each cross
with each filled circle representing one biological replicate; there are three biological replicates per genotype
The numbers at the top represent total seed numbers
The asterisks represent statistical significance as calculated by one-way analysis of variance with post-hoc Tukey’s honestly significant difference test (***P < 0.001)
Upset plot showing the overlap of upregulated genes between interploidy (Cr × 4xCr) and interspecies crosses of different Capsella species
Heat map and dendrogram show clustering of samples based on log2 fold changes (compared with the corresponding maternal parent) of genes upregulated in the analysed hybrids
Source data
These data support the idea that a dosage-sensitive component generated by the maternal parent determines hybridization success
these data strongly suggest that interploidy and interspecies hybridization barriers share a common molecular basis
the fact that increased ploidy of the maternal parent can alleviate paternal-excess hybrid incompatibility implies the existence of a quantitative maternal factor determining hybridization success
Box plots showing methylation levels of TEs in the endosperm of 6 DAP seeds of the indicated genotypes
The asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests; P values were adjusted for multiple comparisons with Benjamini and Hochberg correction (***P < 0.001)
the horizontal lines show the median values
the box edges show the interquartile range and the whiskers show the full range excluding outliers
Source data
these data reveal that interploidy and interspecies hybridization cause similar molecular defects consistent with the similar phenotypes of hybrid seeds
a, DAPI-stained chromocenters from endosperm nuclei from Cr × Cr, Cr × nrpd1, nrpd1 × Cr and nrpd1 × nrpd1. Scale bars, 5 μm. b, Quantification of chromatin condensation given as mean circularity of chromocenters (Methods)
The numbers below the boxes indicate the number of analysed nuclei
The asterisks represent statistical significance as calculated by two-sided Wilcoxon tests; P values were adjusted for multiple comparisons with Benjamini and Hochberg correction (***P < 0.001)
Metagene plots showing DNA methylation levels of TEs in the endosperm of Cr × Cr
The asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests; P values were adjusted for multiple comparisons with Benjamini and Hochberg correction (***P < 0.001; **P < 0.01)
Upset plot showing the overlap of upregulated genes among Cr × 4xCr
Genes were considered as upregulated on the basis of log2(fold change) > 1 and Padj < 0.05 compared with Cr × Cr
Source data
Box plots showing the accumulation of siRNAs (18–25 nucleotides) on siren loci in different genotypes
The asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests (***P < 0.001)
siRNA accumulation and CHH methylation in the endosperm of the indicated genotypes on selected genes overlapping siren loci (marked with violet lines)
The blue boxes represent genes; the purple boxes represent TEs
Parental-specific accumulation of sRNAs on loci having at least 15 parental-specific reads in total
The numbers above the boxes indicate the number of such genes in each genotype
The asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests (***P <0.001)
Parental-specific sRNA accumulation in the endosperm of the indicated genotypes on selected genes
Source data
Comparison of DNA methylation levels in genes (gene body)
promoters and TEs overlapping siren loci with all genes and TEs in the Cr genome
Expression of genes overlapping siren loci in Cr × Cr
The asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests (***P < 0.001; **P < 0.01)
Heat map and dendrogram show clustering of samples based on log2 fold changes (compared with the corresponding maternal parent) of genes overlapping siren loci
Scatter plots showing Pearson’s correlation (r) (two-sided) between the loss of siRNAs and changes in genes expression (left) and CHH methylation (right)
Comparison of DNA methylation in Cr × Cr versus nrpd1 × Cr (left) and Cr × Cr versus Cr × Cg (right) endosperm on upregulated genes (in the respective crosses) overlapping siren loci
The asterisks indicate statistically significant differences as calculated by a two-sided Wilcoxon test (*P < 0.05)
Source data
making it unlikely that reduced NRPD1 expression is causally responsible for the loss of sirenRNAs in the hybrids
CHG and CHH DNA methylation at sirenRNA trans targets (50-bp genomic windows
with ≥1 RPM realigning sirenRNAs and ≤2 mismatches) in Cr × Cr endosperm
The numbers on the plots show the number of windows in each category; the breaking points correspond to 0.7
CHG and CHH DNA methylation at sirenRNA trans targets overlapping genes (coding region +2 kb promoters; top) and TEs (bottom)
The numbers on the plots show the number of windows in each category; the breaking points correspond to 0.5
Comparison of CHG and CHH DNA methylation levels in 50-bp windows differing in sirenRNA accumulation at trans targets
The x axis shows the difference in DNA methylation (Cr × Cr minus Cr × Cg)
and the y axis shows the difference in sirenRNA accumulation in trans (Cr × Cr minus Cr × Cg)
The numbers correspond to windows in each category; the breaking points correspond to 0.6
the asterisks indicate statistically significant differences as calculated by two-sided Wilcoxon tests with Benjamini and Hochberg correction for multiple comparisons (***P < 0.001; *P < 0.05)
Examples of genes and TEs with reduced sirenRNA accumulation at trans targets in Cr × Cg
nrpd1 × Cr and nrpd1 × nrpd1 compared with Cr × Cr endosperm
The tracks show levels of sirenRNAs and CHH methylation at the indicated genes and TEs
Distance to the nearest TE upstream of the transcriptional start site of upregulated genes in Cr × Cg compared with non-upregulated genes
The asterisks indicate statistically significant differences as calculated by a two-sided Wilcoxon test (***P < 0.001)
Methylation levels of TEs in the promoters of upregulated genes in the Cr × Cg hybrid
Statistical differences were calculated with two-sided Wilcoxon’s tests for paired samples
Source data
Distribution of PHE1 binding motifs in the Capsella genome in different groups of genes: all genes and genes upregulated in Cr × Cg
The numbers of pericentromeric (PC) and non-pericentromeric (NPC) genes upregulated in different genotypes are compared with the numbers of all pericentromeric/non-pericentromeric genes
The asterisks indicate statistically significant differences calculated by two-sided chi-square tests with Benjamini and Hochberg correction for multiple comparisons (***P < 0.001)
The numbers show the number of genes in each category
Heat maps and dendrograms show clustering of genes based on the expression (RPKM) of type I γ-MADS-box (b) and α*-MADS-box (c) transcription factors in different Capsella genotypes
Heat map and dendrogram show clustering of genes based on log2(fold change) (in comparison to the maternal parent) of γ and α* type I MADS-box transcription factors in different Capsella hybrids
Genes marked in bold overlap siren loci; genes marked in purple are targeted by trans-acting sirenRNAs
Source data
we propose that seed abortion in response to paternal-excess interspecies and interploidy hybridizations is triggered by two factors: the depletion of maternally derived sirenRNAs and the increased expression of AGLs targeting hypomethylated regions in hybrid endosperm
This strongly implies a direct connection between the depletion of sirenRNAs and the arrest of hybrid seed development
This discrepancy is probably attributed to the amplified AGL expression in the paternal parents of hybrids
inducing a more pronounced response in hybrid endosperm than in the nrpd1 mutant
directly testing the functional relevance of AGLs in establishing interspecies hybridization barriers in Capsella is challenging
but this remains an important task of future studies
we propose that maternal sirenRNAs serve as a dosage-sensitive factor that decisively influences the success of hybridization between plant species
The seeds were surface sterilized with 30% bleach and 70% ethanol
rinsed with distilled water and sown on agar plates containing ½ Murashige and Skoog medium and 1% sucrose
The seeds were then stratified for two days in the darkness at 4 °C and moved into a growth chamber with a long-day photoperiod (16 h and 22 °C light
8 h and 19 °C darkness) with a light intensity of 110 µE
Seven-day-old seedlings were transferred to pots filled with sterile soil
and the plants were grown in a growth chamber with 60% humidity and daily cycles of 16 h light at 21 °C and 8 h darkness at 18 °C with a light intensity of 150 µE
dry seeds were stored for 30 days to break dormancy
The seeds were then surface sterilized and sown on agar plates as described above
The seeds were stratified for two days at 4 °C and then moved to a growth chamber and scored after seven days for seedling establishment
The siliques were opened at the side with needles and incubated overnight in fixing solution (ethanol:acetic acid (3:1)) at 4 °C
The samples were washed with distilled water three times for 15 minutes and then incubated for 1 h in freshly prepared 5 N HCl
the samples were washed again with distilled water three times for 15 minutes and incubated with Schiff reagent (Sigma-Aldrich) for 3–4 h
The samples were washed with cold (4 °C) distilled water three times for 10 minutes and then washed in different concentrations of ethanol (10%
70% and 95%) for 10 minutes in each solution
The samples were then washed with 99.5% ethanol until they remained colourless (at this point samples can be stored in this solution overnight at 4 °C)
The samples were incubated in 99.5% ethanol:LR White (London Resin White + catalyst
The samples were incubated in 1:1 ethanol:LR White for 1 h and then in LR White overnight
mounted on a microscope slide in a drop of LR White + catalyst and baked at 60 °C for 16 h for polymerization
The slides were watched under a two-photon microscope with an excitation wavelength of 800 nm and emission from 518 nm and onwards
DNA was extracted from young leaf material of Cg using the CTAB method45
DNA was sized on the BluePippin system (Sage Science) to remove small fragments and then sequenced on one Oxford Nanopore PromethION flow cell
and the PromethION release version was 19.05.1
corresponding to about 200× coverage of the estimated genome size of approximately 250 Mb (roughly calculated by flow cytometry analysis)
Cg DNA was used to prepare an Illumina overlap library
DNA was sheared using a Covaris M220 (Covaris) to 450 bp
The sheared DNA was sized using a BluePippin prep system and used to prepare a PCR-free Illumina sequencing library
The library was sequenced on the Illumina NovaSeq SP platform using an SP flow cell and 2 ×250 bp protocol
with the default parameters) to generate a haploid representation of the heterozygous Cg assembly
Seeds derived after manual pollination were dissected out of siliques at 6 DAP and collected in 20 µl of RNAlater solution (Sigma-Aldrich)
RNA was extracted using the RNeasy Plant Mini Kit (Qiagen) according to the manufacturer’s instructions
500 ng of RNA was used for RNA-seq library preparation using the NEBNext Poly(A)mRNA Magnetic Isolation Module and NEBNext Ultra RNA LibraryPrep Kit for Illumina
Three biological replicates were generated for each genotype
The libraries were sequenced on an Illumina HiSeq X machine in 150-bp paired-end mode
Manually pollinated seeds 6 DAP were removed from siliques and put on a microscopic slide covered with a piece of tissue paper soaked with a drop of RNAlater solution (Sigma-Aldrich)
The seeds were gently squashed with another microscopic slide to release the endosperm
and the embryos and seed coats were removed with tweezers
Tissue paper with the endosperm was put in an Eppendorf tube and frozen in liquid nitrogen
Approximately 600 seeds were used per replicate
The samples were stored at −70 °C and then used for genomic DNA isolation using the DNeasy Plant Mini Kit (Qiagen)
Biological duplicates were generated for each genotype
Libraries were prepared with the Accel-NGS Methyl-Seq DNA Library Kit from Illumina
and the sequencing was performed on an Illumina NovaSeq 6000 machine in 150-bp paired-end mode
and cytosine methylation values calculated using the Bismark Methylation Extractor
Differentially methylated regions in the CG
CHG and CHH contexts were calculated using 50-bp windows across the genome as units
Only hypomethylated regions (Cr × Cr > Cr × Cg
Cr × Cr > Cr × 4xCr and Cr × Cr > nrpd1 × Cr) were considered
Windows with differences in fractional methylation below the first decile (Fisher’s exact test P < 0.01) were selected
and these were merged if they occurred within 300 bp
Seeds derived after manual pollination were dissected out of siliques at 6 DAP and squeezed on facial tissue paper to release the endosperm
Seed coats and embryos were removed with forceps
A drop of RNAlater solution (Sigma-Aldrich) was added to the tissue containing the absorbed endosperm
transferred to an Eppendorf tube and frozen in liquid nitrogen
Each sample consisted of endosperm from about 600 seeds
Small RNAs were extracted using the mirVana miRNA Isolation Kit (ThermoFisher Scientific) following the manufacturer’s instructions for sRNA
Libraries were prepared using the NEBNext Multiplex Small RNA Library Prep Set for Illumina with 50–100 ng of input for each sample
Size selection was performed on a 6% polyacrylamide gel
and bands corresponding to about 150 bp were cut and purified from the gel for further analysis
Sequencing was performed on a NovaSeq 6000 machine in 150-bp paired-end mode
Adapters were removed from the first read of the 150-bp long read pair of each library using cutadapt
and the resulting 18–25-bp long reads were selected
mitochondria and structural non-coding RNAs (tRNAs
rRNAs or snoRNAs) were removed using bowtie (v.1)
Genes and TEs were considered as depleted of sRNAs on the basis of log2(fold change) < 0 and Padj < 0.1 in comparison to the maternal parent (for incompatible hybrids) or to Cr × Cr (for crosses with the nrpd1 mutant)
we used own-built ‘pseudogenomes’ in which the above-described SNPs between these species and Cr were substituted into the Cr reference genome
Endosperm nuclei spreading was performed as previously described9
Manually pollinated seeds were harvested 4 DAP and incubated overnight in a solution containing 2.5 mM 8-hydroxyquinoline
The seeds were subsequently fixed in ethanol:acetic acid (3:1) for at least five hours at 4 °C
the seeds were washed with 10 mM citrate buffer and incubated for five hours in an enzyme solution comprising 0.3% cytohelicase
0.3% pectolyase and 0.3% cellulase in 10 mM citrate buffer
spread using 60% acetic acid and fixed on the slide with ethanol:acetic acid (3:1)
The slides were mounted using Vectashield mounting medium containing DAPI (BioNordika AB)
The experiment was conducted with three independent biological replicates
Each nucleus was represented by the mean circularity of all chromocenters
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
The role of hybrid seed inviability in angiosperm speciation
Dissection of two major components of the post-zygotic hybridization barrier in rice endosperm
Parent-of-origin effects on seed development in Arabidopsis thaliana
When genomes collide: aberrant seed development following maize interploidy crosses
Manipulations of endosperm balance number overcome crossing barriers between diploid Solanum species
Non-reciprocal interspecies hybridization barriers in the Capsella genus are established in the endosperm
Differences in effective ploidy drive genome-wide endosperm expression polarization and seed failure in wild tomato hybrids
Overcoming the species hybridization barrier by ploidy manipulation in the genus Oryza
Hybrid seed incompatibility in Capsella is connected to chromatin condensation defects in the endosperm
Endosperm evolution by duplicated and neofunctionalized type I MADS-box transcription factors
Paternal easiRNAs regulate parental genome dosage in Arabidopsis
Paternally acting canonical RNA-directed DNA methylation pathway genes sensitize Arabidopsis endosperm to paternal genome dosage
Non-canonical RNA-directed DNA methylation
A small RNA pathway mediates allelic dosage in endosperm
Imprinted expression of genes and small RNA is associated with localized hypomethylation of the maternal genome in rice endosperm
Abundant expression of maternal siRNAs is a conserved feature of seed development
Maternal siRNAs as regulators of parental genome imbalance and gene expression in endosperm of Arabidopsis seeds
RNA Pol IV induces antagonistic parent-of-origin effects on Arabidopsis endosperm
Rice interspecies hybrids show precocious or delayed developmental transitions in the endosperm without change to the rate of syncytial nuclear division
Endosperm-based postzygotic hybridization barriers: developmental mechanisms and evolutionary drivers
Paternally expressed imprinted genes associate with hybridization barriers in Capsella
Divergent mating systems and parental conflict as a barrier to hybridization in flowering plants
The Capsella rubella genome and the genomic consequences of rapid mating system evolution
Hybrid origins and the earliest stages of diploidization in the highly successful recent polyploid Capsella bursa-pastoris
Rapid evolution of genomic imprinting in two species of the Brassicaceae
Maternal components of RNA-directed DNA methylation are required for seed development in Brassica rapa
ShortStack: comprehensive annotation and quantification of small RNA genes
Sorting of small RNAs into Arabidopsis argonaute complexes is directed by the 5′ terminal nucleotide
Ovule siRNAs methylate protein-coding genes in trans
Maternal small RNAs mediate spatial–temporal regulation of gene expression
Endosperm and seed transcriptomes reveal possible roles for small RNA pathways in wild tomato hybrid seed failure
Paternally expressed imprinted genes establish postzygotic hybridization barriers in Arabidopsis thaliana
Auxin regulates endosperm cellularization in Arabidopsis
Parental conflict driven regulation of endosperm cellularization by a family of Auxin Response Factors
The MADS-box transcription factor PHERES1 controls imprinting in the endosperm by binding to domesticated transposons
Structure-based discovery and description of plant and animal Helitrons
Helitron distribution in Brassicaceae and whole genome Helitron density as a character for distinguishing plant species
Polymerase IV plays a crucial role in pollen development in Capsella
Nurse cell-derived small RNAs define paternal epigenetic inheritance in Arabidopsis
maintaining and modifying DNA methylation patterns in plants and animals
Mating system is associated with seed phenotypes upon loss of RNA-directed DNA methylation in Brassicaceae
Endosperm cellularization defines an important developmental transition for embryo development
Parent-dependent loss of gene silencing during interspecies hybridization
Separating phases of allopolyploid evolution with resynthesized and natural Capsella bursa-pastoris
Minimap2: pairwise alignment for nucleotide sequences
Minimap and miniasm: fast mapping and de novo assembly for noisy long sequences
FLASH: fast length adjustment of short reads to improve genome assemblies
Fast and accurate short read alignment with Burrows–Wheeler transform
Pilon: an integrated tool for comprehensive microbial variant detection and genome assembly improvement
Identifying and removing haplotypic duplication in primary genome assemblies
Graph-based genome alignment and genotyping with HISAT2 and HISAT-genotype
featureCounts: an efficient general purpose program for assigning sequence reads to genomic features
Moderated estimation of fold change and dispersion for RNA-seq data with DESeq2
Long-term balancing selection drives evolution of immunity genes in Capsella
Bismark: a flexible aligner and methylation caller for bisulfite-seq applications
SNPsplit: allele-specific splitting of alignments between genomes with known SNP genotypes
Garrison, E. & Marth, G. Haplotype-based variant detection from short-read sequencing. Preprint at https://arxiv.org/abs/1207.3907 (2012)
BEDTools: a flexible suite of utilities for comparing genomic features
HTSeq—a Python framework to work with high-throughput sequencing data
Improved placement of multi-mapping small RNAs
Ultrafast and memory-efficient alignment of short DNA sequences to the human genome
Fiji: an open-source platform for biological-image analysis
Genetic dissection of morphometric traits reveals that phytochrome B affects nucleus size and heterochromatin organization in Arabidopsis thaliana
Recruitment of the histone variant macroH2A1 to the pericentric region occurs upon chromatin relaxation and is responsible for major satellite transcriptional regulation
Identification of the elementary structural units of the DNA damage response
Simple combinations of lineage-determining transcription factors prime cis-regulatory elements required for macrophage and B cell identities
Dziasek, K. et al. Dosage sensitive maternal siRNAs determine hybridization success in Capsella. figshare https://doi.org/10.6084/m9.figshare.27143508 (2024)
Efficient test and visualization of multi-set intersections
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Lascoux from Uppsala University for kindly sharing tetraploid Co seeds
Bente for valuable suggestions about sRNA library preparation and M
Incarbone and members of the Köhler group for critical reading and helpful comments on the paper
This work was funded by the Knut and Alice Wallenberg Foundation (grant numbers 2018-0206 (C.K.) and 2019-0062 (C.K.)) and the Max Planck Society
Open access funding provided by Max Planck Society
Swedish University of Agricultural Sciences and Linnean Centre for Plant Biology
Department of Plant Reproductive Biology and Epigenetics
Max Planck Institute of Molecular Plant Physiology
developed the methodology and provided supervision
generated the genetic material used in this study
acquired the funding and administered the project
Nature Plants thanks the anonymous reviewers for their contribution to the peer review of this work
Germination of triploid Cr seeds shown as the fraction of germinating seeds from each cross
Each filled circle represents one biological replicate; there are three biological replicates per genotype
Numbers on top represent total seed number
Asterisks represent statistical significance as calculated by one way ANOVA with post hoc Tukey’s HSD test (*** p < 0.001)
Red dots show values for three biological replicates
Whiskers show the full range excluding outliers
Feulgen staining of diploid and triploid Cr seeds at 6 DAP (scale bars represent 200 µm)
Cr × 4xCr embryos rescued on Murashige-Skoog medium
Upset plot showing the overlap of upregulated genes in comparison to the paternal parent (e) and both parents (f) between interploidy (Cr × 4xCr) and interspecies crosses of different Capsella species
Source data
Metagene plots show DNA methylation levels of genes in the endosperm of Cg × Cg
Boxplots show methylation level of genes in the endosperm of Cg × Cg
Asterisks indicate statistically significant differences as calculated by the two-sided Wilcoxon test
p-values were adjusted for multiple comparisons with Benjamini and Hochberg correction (** p-value <0.01,*** p-value < 0.001
Metagene plots show DNA methylation levels of genes in the endosperm of Cg × Cr at 6 DAP in comparison to published data for Cr × Cr
Boxplots show methylation level of genes in the endosperm Cg × Cr at 6 DAP in comparison to published data for Cr × Cr
p-values were adjusted for multiple comparisons with Benjamini and Hochberg correction (*** p-value < 0.001)
Metagene (e) and box plots (f) show DNA m2ethylation levels of genes in the endosperm of diploid and triploid 6 DAP Cr seeds
Metagene (g) and box plots (h) show DNA methylation levels of TEs in the endosperm of diploid and triploid 6 DAP Cr seeds
Boxplots show CHG (left panel) and CHH (right panel) methylation levels on TEs in chromosome arms and pericentromeric regions in the endosperm of Cr × Cr
Cr × Cg and Cg × Cg and Cr × 4xCr at 6 DAP
Asterisks indicate statistically significant differences as calculated by the two-sided Wilcoxon test (*** p-value < 0.001)
Boxes show median values and the interquartile range
Source data
Metagene (a) and box plots (b) show DNA methylation levels of TEs in the endosperm of Cr × Co
Metagene (c) and box plots (d) show DNA methylation levels of TEs in the endosperm of Cr × Co
Source data
Source data
Barplot shows number of aborted and partially aborted seeds of three biological replicates of each genotype
Numbers above the bars indicate number of analysed seeds
Pictures of cleared seeds of Cr × Cr and nrpd1 × Cr at 6 DAP
Inset shows enlarged regions of cellularized (Cr × Cr) and uncellularized (nrpd1 × Cr) endosperm
Scale bars represents 100 µm (upper row) and 10 µm (lower row)
Quantification of endosperm cellularization of indicated genotypes at 6 DAP
Numbers correspond to numbers of analysed seeds
Seed phenotypes of 4xCr × Cg and 4xnrpd1 × Cg seeds
Barplot shows number of aborted and partially aborted and viable seeds of three biological replicates of each genotype
Seed phenotypes of Cr × 4xCr and Cr × 4xnrpd1 seeds
Source data
Non-metric MultiDimensional Scaling (NMDS) of small RNA (sRNA) sequencing samples
Correlogram showing the correlation score matrix across all sequenced sRNA libraries
Barplot shows size distribution of sRNAs in all sequenced libraries
Siren loci are larger than other siRNA expressing loci
Genomic features overlapping with 24 nt-dominant clusters (n=28 075) and siren loci (n=1 385) in Cr
The genome was subdivided into 50-bp windows (n= 2 497 626) that were assigned to either exons
transposable elements and edges (50bp regions at the boundaries of gene bodies and repeats)
Frequency distribution of sirenRNA clusters after dominating size class
24 nt siRNAs dominate in the majority of sirenRNA clusters defined by ShortStack
5′ nucleotide of sirenRNAs (18–24 nt) in Cr × Cr endosperm
Number of siren loci normalized per size of respective genomic regions (in bp) – non-pericentromeric and pericentromeric for each of the eight Cr chromosomes
Distribution of siren loci along the eight chromosomes of the Cr genome
black boxes indicate positions of pericentromeric regions
TE families overlapping with24 nt-dominant and siren loci compared to the genome-wide frequencies in Cr
Source data
siRNA accumulation and CHH methylation in the endosperm of indicated genotypes on selected genes overlapping siren loci: Carubv10025009m.g (AGL33)
Boxplots show DNA methylation on γ and α* type I MADS box TFs in 6 DAP endosperm of different Capsella genotypes
Asterisks indicate statistically significant differences as calculated by the two-sided Wilcoxon test for paired samples
p-values were adjusted with Benjamini and Hochberg correction (*** p-value < 0.001
Barplot shows log2 fold change expression level of indicated genes in comparison to respective maternal plants
Asterisks indicates statistical significance as calculated with Wald test in DESEQ2 (*** padj < 0.001
Source data
Boxplot show parental-specific DNA methylation levels of genes (a) and TEs (b) in the endosperm of Cr × Cg
Maternal and paternal methylation values in each genotype are compared to the respective parent in the Cr × Cg cross
p-values were adjusted for multiple comparisons with Benjamini and Hochberg correction (p-value: ***< 0.001
Boxplot show parental-specific DNA methylation levels of genes (c) and TEs (d) in the endosperm of Co × Cr
Maternal and paternal methylation values in each genotype are compared to the respective parent in Co × Cr cross
Source data
Heatmaps show expression of AGL genes (RPKM) targeted by trans-acting sirenRNAs
accumulation of sirenRNAs at trans AGL targets and corresponding CHG and CHH methylation
Tracks show sirenRNA accumulation at trans AGL targets and corresponding CHH and CHG methylation levels (same set of genes as on panel a)
The purple line above the tracks marks cis acting siren RNAs
Light green and navy-blue bars on sirenRNA tracks show reads mapping in cis at siren loci
Barplots show the proportion of maternal and paternal reads in genes upregulated in Cr × Cg (c)
γ-type AGLs upregulated in Cr × Cg (d) and selected orthologs of genes that have been previously reported as imprinted and involved in endosperm development or the triploid block in Arabidopsis (e)
Expression data are obtained from whole seeds at 6 DAP
Black horizontal line on each plot represents the expected 2:1 ratio (maternal:paternal) for biallelic genes in the endosperm
Boxplot show the ratio of paternal:maternal read counts for all genes and genes upregulated in Cr × Cg
Source data
The table shows log2 fold changes of gene expression in the endosperm of the indicated crosses
List of siren loci and overlapping genomic features
The table shows the positions and normalized read counts over siren loci in the endosperm of the indicated genotypes
List of potential trans targets affected in the Cr × Cg hybrid
The table shows differences in sirenRNA accumulation (Diff_RPM > 0)
differences in CHH and CHG methylation (diff_CHH > 0.01 OR diff_CHG > 0.05)
and differences in RNA accumulation (log2 fold change > 1
p < 0.05) in Cr × Cg compared with Cr × Cr
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DOI: https://doi.org/10.1038/s41477-024-01844-3
Karen O’Leary is an Associate Research Analysis Editor with Nature Medicine
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This article is part of the Research TopicNanotechnology and Nanoscience to manage SARS-CoV-2 Variants of ConcernView all 14 articles
Small interfering RNA (siRNA)-mediated mRNA degradation approach have imparted its eminence against several difficult-to-treat genetic disorders and other allied diseases
Viral outbreaks and resulting pandemics have repeatedly threatened public health and questioned human preparedness at the forefront of drug design and biomedical readiness
During the recent pandemic caused by the SARS-CoV-2
mRNA-based vaccination strategies have paved the way for a new era of RNA therapeutics
RNA Interference (RNAi) based approach using small interfering RNA may complement clinical management of the COVID-19
RNA Interference approach will primarily work by restricting the synthesis of the proteins required for viral replication
thereby hampering viral cellular entry and trafficking by targeting host as well as protein factors
the stability of small interfering RNA in the physiological environment is of grave concern as well as site-directed targeted delivery and evasion of the immune system require immediate attention
nanotechnology offers viable solutions for these challenges
The review highlights the potential of small interfering RNAs targeted toward specific regions of the viral genome and the features of nanoformulations necessary for the entrapment and delivery of small interfering RNAs
In silico design of small interfering RNA for different variants of SARS-CoV-2 has been discussed
Various nanoparticles as promising carriers of small interfering RNAs along with their salient properties
This review will help tackle the real-world challenges encountered by the in vivo delivery of small interfering RNAs
and readily available drug candidate for efficient management of SARS-CoV-2 in the future
The review equivocally concludes the significance of siRNA-based nanoparticle formulation as a better alternative against SARS-CoV-2
the study did not consider any in vivo delivery approach
Whether targeting viral or host targets are more effective (preferable) is an open question
siRNA guide strand sequences reported in literature along with their target site
FIGURE 2. Computational pipeline to predict siRNA against target segments of SARS-CoV-2. Adapted with modifications from Ref. (Chowdhury et al., 2021)
Some of the potential nanocarriers are briefly discussed in this section
FIGURE 3. Potential nanocarrier configurations for siRNA delivery. The carriers can be categorized into organic (i.e., derived from lipid, polymeric and polysaccharides) and inorganic types. The size and structural features of these nanocarriers are depicted. Adapted from Ref. (Zhang et al., 2022a)
PEGylated lipids and cholesterol) used for lipid nanoformulations
FIGURE 5. The ionization characteristics of the commercially available ILs obtained through zeta potential measurement. The LNPs showed a transition of charges-positive zeta potential at low pH and negative zeta potential at high pH, covering the range of endosomal and lysosomal pH. Adapted from Ref. (Carrasco et al., 2021)
The degraded fragments of the lipids are rapidly cleared from the body allowing for multiple doses within a short duration
The prepared lipidoid CS12-200 nanoparticles showed 83.8% siRNA loading when formulated with or without PEGylated helper lipids
The transfection efficacy for siRNA on neural cells was also increased twice without toxicity
the suitability of lipidoids for the delivery of siRNA for various purposes can be explored
FIGURE 6. Folate incorporated liposome formulation for gene silencing applications. siRNA for Mcl-1 (a protein expressed in the rheumatoid joint macrophages) silencing was loaded in liposome and targeted towards folate receptor. PEGylated liposome offered stealth features against phagocytic uptake; neutral lipids exhibited low toxicity while specific targeting was observed by anchoring folate-targeted peptides. Adapted from Ref. (Nogueira et al., 2017)
The γ-[32P]-ATP labeled siRNA was efficiently transfected in three different xerographs without exhibiting toxicity
The knockdown efficacy in H441-luc cells due to the polymer-tyrosine-siRNA complex was also found efficient
proving the capabilities of polymeric nanoparticles for siRNA delivery
The schematic of an IL illustrating the main elements and how they contribute towards stability
FIGURE 9. Schematic illustration of the stability of LNPs based on size. Adapted from Ref. (Sato et al., 2016)
ALN-0319 (adapted from ref 113) L3 (adapted from ref 112) CL4H6 (adapted from ref 111) with cleavable ester linkage sites (highlighted in blue color) and expected hydrolysis pathway catalyzed by esterases
Better understanding and control of the LNP fate in vivo is important and this has been actively explored in numerous studies
Algarni et al. have explored the targeting efficiency of three ionizable cationic lipids, DLin-MC3-DMA, DLin-KC2-DMA and DODAP (1,2-dioleoyl-3-dimethylammonium-propane), for the organ-specific delivery of pDNA (Algarni et al., 2022)
The intravenous administration in mice models with LNPs formulations showed that the DLin-MC3-DMA and DLin-KC2-DMA bearing LNPs more precisely and efficiently transfected the nucleic acid cargo to the spleen instead of the liver
DLin-MC3-DMA and DLin-KC2-DMA with two double bonds per alkyl chains
has influenced the transfection efficiency in the spleen
the selection of suitable ILs may improve the targeting
The LNP contained DMKE (45%) (O,O′-dimyristyl-N-lysyl glutamate)
and was prepared by a methanol and chloroform mixture (2:1
FIGURE 11. (A) The structure of aptamer molecules conjugated onto LNP-RNAi complex. LNPs were first complexed with siRNAs, which were then conjugated with synthesized aptamers. (B) SELEX-based method for aptamer selection after multiple rounds of binding, separation, washing, elution and amplification. Adapted from ref. (Saify Nabiabad et al., 2022)
the in vitro and in vivo targeting aspects of these aptamers are yet to be verified
(A) Preparation of SORT LNPs for mRNA delivery for liver
spleen and lungs by incorporation of different SORT lipids in the formulation of LNPs
(B) The level of luciferase expression after administration of 5A2-SC8 SORT LNPs in mice models
With the increased cationic lipid DOTAP percentage
the expression of luciferase shifted from liver to spleen to lungs
Effects of incorporation of SORT molecules in LNPs formulations visible from luminescence profile for tested mice models. Adapted from Ref. (Cheng et al., 2020)
further bursting of endosomes releasing the siRNA in the cytoplasm following the complete disintegration of LNP structure during the process
the fast mutation rate of the viral genome has to be kept in mind with potentially targeting the conserved viral domains with the help of available libraries and computational resources
Approved and under trial siRNA therapeutics for different diseases
Considering the ever-changing dynamic mutations in the SARS-CoV-2 genome
the demand for well-targeted specific and highly effective therapeutics are needed
Genomic regions of the virus conserved across the variants and sub-variants could be first targeted to inhibit viral entry and replication in the host
Many in silico algorithms and web servers have been deployed to design siRNAs following the three golden rules of design
The accessory parameters such as heat capacity (CP)
and off-target matches are predicted computationally
some validation efforts have been attempted to experimentally verify the silencing efficiency of the computationally designed siRNAs
but this will require more extensive studies to assure confidence in the theoretical designs
a handful of effective designs are now available that could be tested in a clinical setting
should there be sufficient impetus from clinicians and industrial parties
the designed siRNAs can be formulated with different nanocarriers for practical utility
Lipids-based and polymeric nanoparticles offer the flexibility of conjugation with siRNAs and surface functionalization for targeted delivery
siRNAs-based therapies have been approved for other diseases
but in the case of COVID-19 clinical trials are yet to be undertaken
Along with the efficacy of nano-formulations
other inflammatory responses should be investigated through in vivo studies
excessive inflammation that is ultimately cause of patient exhaustion in clinic
The dosage of siRNAs should be confined to a minimum concentration
preferably below 100 nM at local sites and <1 mg/kg overall for practical translation of delivery systems
The siRNA-based nano-formulations appear to be promising for the therapy of contagious COVID-19 and post-COVID inflammations
and LP drafted the manuscript and LP and HU edited the manuscript
The authors acknowledge the Shastri Indo-Canadian Institute for the Shastri COVID-19 Pandemic Response Grant (SCPRG) 2020-21 for financial assistance for this work
The studies in HU’s lab are supported by NSERC
NFRF and project support by MITACS/RJH Biosciences
HU has ownership interest in materials that could be used in siRNA delivery
AR was supported by a MITACS fellowship sponsored by RJH Biosciences
The remaining authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest
All claims expressed in this article are solely those of the authors and do not necessarily represent those of their affiliated organizations
Any product that may be evaluated in this article
or claim that may be made by its manufacturer
is not guaranteed or endorsed by the publisher
Transactivation response RNA-binding protein; SARS-COV 2
Severe acute respiratory syndrome coronavirus 2; LNP
(6Z,9Z,28Z,31Z)-heptatriacont-6,9,28,31-tetraene-19-yl 4-(dimethylamino)butanoate; ALC-0315
[(4-hydroxybutyl)azanediyl]di(hexane-6,1-diyl) bis(2-hexyldecanoate); SM-102
(1-Octylnonyl 8-[(2-hydroxyethyl)[6-oxo-6(undecyloxy)hexyl]amino]-octanoate); DOPE
1,2-dioleoyl-3-dimethylammonium-propane; RBD
Systemic Evolution of Ligands by EXponential enrichment; DMKE
O,O′-dimyristyl-N-lysyl glutamate; SORT
Dioleoyl-3-trimethylammonium propane; hATTR
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Received: 30 November 2022; Accepted: 13 January 2023;Published: 06 February 2023
Copyright © 2023 Fopase, Panda, Rajendran, Uludag and Pandey. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use
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*Correspondence: Lalit M. Pandey, bGFsaXRwYW5kZXlAaWl0Zy5hYy5pbg==; Hasan Uludag, aHVsdWRhZ0B1YWxiZXJ0YS5jYQ==
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RNA interference (RNAi) is a promising gene-silencing technique for pest control that targets essential genes
We assessed the potential of double-stranded RNA (dsRNA) and small interfering RNA (siRNA) to silence mesh or iap genes in the midguts of Spodoptera litura larvae
Despite the theoretical promise of RNAi approaches
our findings revealed that dsRNA did not induce significant gene silencing or impact larval growth
whereas siRNA exhibited clear insecticidal effects
likely by disrupting intestinal osmoregulation and impairing larval fitness
Detailed analysis indicated that dsRNA could not be efficiently converted into functional siRNA in the midguts of S
possibly due to the low expression levels of Dicer-2 and the rapid degradation of dsRNA within the gut environment
while dsRNA demonstrated greater environmental stability than siRNA under soil conditions
litura to process dsRNA effectively limits its viability as a pest control agent
These findings indicate the critical role of Dicer-2 in RNAi-mediated gene silencing and highlight the challenges and limitations of employing dsRNA-based genetic pesticides in lepidopteran species
the efficacy of dsRNA-based pesticides in controlling lepidopteran pests
we assume that targeting mesh could reduce the integrity and normal function of larval digestive system and causing mortality
Our findings indicate that the low expression of Dicer-2
coupled with the rapid degradation of dsRNA in the gut environment of S
significantly impedes the conversion of dsRNA into functional siRNA
thereby rendering dsRNA-based pest control strategies ineffective in this species
These results highlight the importance of further research aimed at improving dsRNA stability and enhancing conversion efficiency in lepidopterans
may offer a more effective approach for pest management in S
Total RNA was isolated from various larval instars using TRIzol reagent (Invitrogen), following the manufacturer’s instructions. A NanoDrop OneC spectrophotometer (Thermo Fisher Scientific) was used to determine the RNA concentration. cDNA was synthesized from 500 ng of total RNA using the PrimeScript RT Reagent Kit (TaKaRa) following the manufacturer’s instructions. cDNA was diluted 10-fold for subsequent experiments (14)
Double-stranded RNA (dsRNA) targeting the mesh and iap genes was synthesized using gene-specific primers designed via the Primer-BLAST tool (NCBI)
The primer sequences for Mesh were 5’-CGC TTC TCA AGT GTG GGT CT-3’ (forward) and 5’-TGA CCT GAC CGT GGA TGT TG-3’ (reverse)
while those for iap were 5’-CCG TGG AGA TGA AGT CCG TT-3’ (forward) and 5’-CCC AGG GTA CGT CAT GGT TC-3’ (reverse)
A mesh or iap gene fragment was PCR-amplified using “Fermentas” under the following conditions: 5 min at 96°C; 40 cycles at 96°C for 30 s
and 72°C for 20 s; and a final extension at 72°C for 3 min
the PCR product was used as a template for the second round of PCR to add T7 promoter sequences to both ends
A GenepHlow gel/PCR kit (Geneaid) was used to purify the resulting product
The MEGAscript T7 Kit (Invitrogen) was used to synthesize dsRNA against the mesh or iap genes
following the manufacturer’s instructions
TURBO DNase digestion removed the template DNA
and dsRNA was recovered using TRIzol reagent
The quality and quantity of dsRNA were assessed by electrophoresis on a 1% agarose gel and spectrophotometry
Taiwan conducted a mesh or iap gene sequence analysis for siRNA synthesis and further predicted and synthesized three siRNA sequences
The primer of candidate genes for analysis gene expression
Total protein from the dissected midgut of S
litura was extracted by homogenization in 60 µL 1× RIPA solution (Bio Basic Inc.
followed by 20 min of ice incubation and centrifugation at 1,000 ×g for 10 min to remove debris
The samples (20 µL each) were mixed with an equal volume of 4× Laemmli Sample Buffer (Bio-Rad
The samples were subsequently incubated at 99°C for 10 min and stored at −20°C until use
Electrophoresis was performed using the Mini-PROTEIN Tetra System (Bio-Rad) and PowerPac Basic (Bio-Rad)
Protein samples (20 µL) and 5 µL of AccuRuller RGB Pre-stained Protein Ladders (Omics Bio
Taiwan) were resolved on a 10% sodium dodecyl sulfate-polyacrylamide gel and transferred onto an Immobilon Transfer Membrane (Millipore
The membrane was blocked with 5% bovine serum albumin (UniRegion Bio-Tech
Taiwan) in Tris-buffered saline with 0.1% Tween 20 (VWR Life Science AMRESCO
U.S.) and subsequently incubated with rabbit polyclonal anti-Dicer-2 (1:5000; Abcam ab4732) and mouse monoclonal actin primary antibodies (1:2500; Yao-Hung Biotechnology Inc.
This was followed by a 1-h incubation with horseradish peroxidase-conjugated goat anti-rabbit secondary antibody (1:1000; Millipore) for the anti-Dicer-2 antibody and goat anti-mouse secondary antibody (1:1000; Millipore) for the actin antibody at 26°C
The signal was detected using UVP Chemostudio (Analytik Jena)
Differential RNAi-mediated silencing of the mesh gene and its impact on Spodoptera litura larval mortality
(A) Expression of the mesh gene in the midgut of Spodoptera litura larvae 24 hours after feeding with dsRNA or siRNA
The control group was fed with siRNA targeting the egfp gene
(B) Larval mortality assessed 12 days after feeding with 0.3 μg of dsMESH or siMESH
Data represent the mean ± standard deviation from three independent experiments
Differences between experimental groups were analyzed using Student’s t-test
Effect of dsRNA injection and feeding on Spodoptera litura
(A) qPCR analysis of mesh gene expression 24 hours after injecting 0.3 μg dsRNA per individual
The control group was injected with dsRNA targeting the egfp gene
(B) qPCR analysis of mesh gene expression in the midgut 24 hours after feeding with 0.3 μg dsRNA per individual
Expression levels in the control group were set to 100%
Three biological replicates were performed
Statistical differences between groups were evaluated using Student’s t-test
with significance defined as p < 0.05 (*)
To verify that the difference in RNAi efficiency between dsRNA and siRNA feeding is not gene-specific, we conducted an additional experiment targeting a second gene, the inhibitor of apoptosis protein (iap). Similar results were observed, showing that siRNA feeding significantly suppressed gene expression (Figure 3A) and induced higher mortality (Figure 3B) compared to dsRNA feeding
Enhanced insecticidal effect of siRNA Targeting the iap Gene in Spodoptera litura larvae
(A) Expression of the iap gene in the midgut of S
litura larvae 24 hours after feeding with dsRNA or siRNA
(B) Impact of dsIAP and siIAP feeding on larval survival over 12 days
larvae were fed 0.3 μg of dsRNA or siRNA per individual per day for four consecutive days
While the same mass of dsRNA and siRNA was used
their molar amounts differ due to the shorter length of siRNA
resulting in a higher molar concentration compared to dsRNA
Statistical significance was indicated as p< 0.05 (*)
Conversion Efficiency of dsRNA into siRNA and Expression Levels of RNAi-Related Genes in the Midgut of S
(A) Northern blot analysis showing the conversion of dsRNA into siRNA in S
Small RNA was extracted from the midgut at various time points (2
12 and 24 hours post feeding) following dsRNA ingestion
C: Synthesized small RNA was directly loaded onto a gel as an untreated control
(B) qRT-PCR analysis of key genes involved in the processing of long dsRNA into siRNA in the midguts of 2nd to 4th instar S
Ago2-X1 and Ago2-X2 represent alternative splicing isoforms of Ago2
The scale bar indicated -ΔΔCT value subtracted by Dicer2 in each instar
The number in each cell represented the average and standard deviation (n=5)
This low dicer-2 expression may explain the failure of dsRNA to effectively trigger RNAi in the midgut
suggesting that reduced dicer-2 expression may be an important factor in the inefficient RNAi response
Reduced Dicer-2 expression in the midgut of Spodoptera litura larvae impairs the conversion of double-stranded RNA (dsRNA) into small interfering RNA (siRNA)
(A) qRT-PCR analysis was performed to measure the expression levels of the dicer-2 gene in the midguts of various insect species
The expression level of 18S rRNA was independently quantified for each species and standardized to 100%
The relative expression levels of the dicer-2 gene were normalized against this baseline
Statistical differences between experimental groups were analyzed using Student’s t-test
Statistical significance was indicated as p < 0.01 (**)
(B) Western blot analysis confirming Dicer-2 expression in the midgut of S
Anti-actin antibodies were used as a loading control
Total protein was extracted from the midgut tissue
qRT-PCR analysis of dsRNA degradation in midgut fluid from S
Midgut juice was extracted from a single larva per biological replicate
The gut juice from one larva was mixed with PBS (1:10 dilution) before incubating with 40 μg of dsRNA
Degradation was analyzed at 30 and 60 minutes using qRT-PCR
The y-axis represents the relative transcript abundance
A relative transcript abundance of 0 indicates undetectable dsRNA levels
The experiment was conducted with four biological replicates
These findings indicate that the failure of dsRNA to function in S
litura is due to both low Dicer-2 expression
these physiological limitations suggest that dsRNA-based pesticides are unlikely to be effective against S
Impact of double-stranded RNA (dsRNA) and small interfering RNA (siRNA) on Spodoptera litura larvae
whereas siRNA demonstrates notable toxicity against the larvae
litura is attributed to the absence of key genes in the midgut necessary for processing dsRNA into siRNA
These findings indicate the limitations of dsRNA in S
litura due to inefficient RNAi processing and rapid degradation in the midgut
particularly with the potential for formulation improvements that improve stability and uptake in pest species resistant to traditional RNAi approaches
The raw data supporting the conclusions of this article will be made available by the authors
The manuscript presents research on animals that do not require ethical approval for their study
The author(s) declare that financial support was received for the research and/or publication of this article
This research was funded by the grant MOST111-2313-B-002-038-MY3 to Y-LW from the Ministry of Science and Technology
Alexander Barton for kindly revising the manuscript
The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest
The author(s) declare that no Generative AI was used in the creation of this manuscript
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A nuclease specific to lepidopteran insects suppresses RNAi
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Lin Y-H and Wu Y-L (2025) Differential RNAi efficacy of siRNA and dsRNA targeting key genes for pest control in Spodoptera litura
Received: 11 February 2025; Accepted: 01 April 2025;Published: 30 April 2025
Copyright © 2025 Lin, Lu, Liu, Su, Lin and Wu. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY)
*Correspondence: Yu-Hsien Lin, eS5oLmxpbkB1dmEubmw=; Yueh-Lung Wu, cnVud3VAbnR1LmVkdS50dw==
†These authors have contributed equally to this work
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small-interfering RNAs (siRNAs) mediate epigenetic silencing via the RNA-directed DNA methylation (RdDM) pathway
which is particularly prominent during reproduction and seed development
there is limited understanding of the origins and dynamics of reproductive siRNAs acting in different cellular and developmental contexts
we used the RNaseIII-like protein RTL1 to suppress siRNA biogenesis in Arabidopsis pollen
and found distinct siRNA subsets produced during pollen development
We demonstrate that RTL1 expression in the late microspore and vegetative cell strongly impairs epigenetic silencing
and resembles RdDM mutants in their ability to bypass interploidy hybridization barriers in the seed
germline-specific RTL1 expression did not impact transgenerational inheritance of triploid seed lethality
These results reveal the existence of multiple siRNA subsets accumulated in mature pollen
and suggest that mobile siRNAs involved in the triploid block are produced in germline precursor cells after meiosis
or in the vegetative cell during pollen mitosis
but the biological significance of this mechanism remains poorly understood
By using two pollen-specific promoters with very different expression dynamics
we were able to identify distinct TE-derived siRNA subsets produced during pollen development
and demonstrate that RTL1 expression in pollen impairs epigenetic silencing to promote triploid seed viability in the next generation
a Schematic representation of RTL1 expression in mature pollen driven by the pLAT52 and pMGH3 promoters that are preferentially expressed in the vegetative cell and sperm cells
b Principal component analysis after variance-stabilizing transformations shows reproducibility of small RNA sequencing experiments for two independent transgenic lines of each construct and wild-type Col-0
and highlights variance along PC1 and PC2 between all sample types
c Heatmap representation of siRNA depletion in pLAT52::RTL1 and pMGH3::RTL1 pollen (vs WT Col-0) shows that distinct loci are affected in the two transgenic lines
d Barplots present examples of different protein-coding genes showing reduced levels of 21/22-nt siRNA in pLAT52::RTL1 or in pMGH3::RTL1 pollen
Dots and bars represent expression level of individual replicates and mean values (n = 2)
a Comparative small RNA analysis between transgenic and WT Col-0 pollen shows that siRNA depletion in pLAT52::RTL1 and pMGH3::RTL1 pollen occurs primarily at TEs
Among all TEs annotated in the Arabidopsis TAIR10 genome
the LTR/Gypsy superfamily was found over-represented in the lists of differentially expressed siRNA loci
b Different members of the LTR/Gypsy superfamily showed significantly reduced siRNA levels in pLAT52::RTL1 or pMGH3::RTL1 pollen
The bar plots show the fraction of TE superfamilies in the two datasets
c Many retrotransposons from the ATGP1 family lost siRNAs specifically in pLAT52::RTL1 pollen
while ATGP2 and ATGP2N lost siRNAs specifically in pMGH3::RTL1 pollen
The bar plots show the fraction of TE families in the two datasets
d siRNAs depleted in pLAT52::RTL1 or pMGH3::RTL1 pollen are dependent on Pol IV activity
c Genome browser tracks show CHH methylation (green) and RNA sequencing (black) datasets at selected loci
Partial CHH hypomethylation is observed specifically in nrpd1a-3FTL and pLAT52::RTL1 pollen
leading to the transcriptional activation of retrotransposons
d RNA sequencing confirmed RTL1 expression in both pLAT52::RTL1 and pMGH3::RTL1 pollen
but up-regulation of LTR/Gypsy retroelements from the ATHILA4A
ATHILA4 and ATGP1 families occurs only in pLAT52::RTL1 and nrpd1a-3FTL pollen
and normalized expression values were calculated by DESeq2 using the median of ratios method
Source data are provided as a Source Data file and in Supplementary Data 2
a The triploid block response in jas-3 mutants is quantified by counting the number of collapsed seeds in six siliques of selfed plants
which reflects the amount of diploid pollen produced in this mutant background (30 to 40%)
Seed abortion is significantly reduced in jas-3/nrpd1a-3 double mutant plants in the F3 generation
and also across five consecutive generations of three independent jas-3;pLAT52::RTL1 lines
while jas-3;pMGH3::RTL1 remains similar to jas-3 controls
Numbers above each box represent the number of individual plants used for each genotype
and their levels of triploid seed collapse is represented by the dots on top of each box
Boxes represent the interquartile range (IQR) showing the lower (Q1) and upper (Q3) quartiles surrounding the median (central line)
and whiskers represent the minimum (Q1 –1.5*IQR) and maximum (Q3 + 1.5*IQR) values
Statistically significant differences in the percentage of collapsed seeds were calculated by ANOVA with a post hoc Dunnett test
using jas-3 as the reference group (ns is not significant
b Representative images of seeds show lower levels of seed abortion in suppressor lines jas-3/nrpd1a-3 and jas-3;pLAT52::RTL1
in comparison with a non-suppressor line jas-3;pMGH3::RTL1 and jas-3 controls
It is tempting to speculate that a subset of germline small RNAs is part of a surveillance mechanism that is primed to act only in situations of epigenetic instability caused by stress or hybridizations that lead to bursts of TE expression and activity
These outstanding questions may now be tested by using RTL1-mediated suppression of sperm siRNAs in different plant species and developmental contexts
Transgenic seeds were surface sterilized with 50% bleach followed by 70% ethanol for 2 min
washed with sterile deionized water and sowed on agar plates (0.5X MS medium
pH 5.7) supplemented with cefotaxime (250 mg/L
Plates were placed in a growth chamber at 23 °C
120 μE m–2 light with a 16-h light/8-h dark (long days) photoperiod for two weeks
and seedlings were then transferred to soil and grown in greenhouse long-day conditions to complete the life cycle (16 h light and 8 h dark)
MGH3 and ACT2 were used as internal controls
Approximately 500,000 pollen grains of each population were used for downstream analysis
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article
Vaucheret, H. & Voinnet, O. The plant siRNA landscape. Plant Cell https://doi.org/10.1093/plcell/koad253
Chow, H. T. & Mosher, R. A. Small RNA-mediated DNA methylation during plant reproduction. Plant Cell https://doi.org/10.1093/plcell/koad010
Epigenetic control of transposons during plant reproduction: From meiosis to hybrid seeds
Small RNAs: big impact on plant development
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mediator of paramutation1 is required for establishment and maintenance of paramutation at multiple maize loci
Life after meiosis: patterning the angiosperm male gametophyte
Reprogramming of DNA methylation in pollen guides epigenetic inheritance via small RNA
Active DNA demethylation in plant companion cells reinforces transposon methylation in gametes
Epigenetic reprogramming and small RNA silencing of transposable elements in pollen
Transposon-derived small RNAs triggered by miR845 mediate genome dosage response in Arabidopsis
The miRNome function transitions from regulating developmental genes to transposable elements during pollen maturation
Loss of small-RNA-directed DNA methylation in the plant cell cycle promotes germline reprogramming and somaclonal variation
Silencing in sperm cells is directed by RNA movement from the surrounding nurse cell
Wu, W. et al. Heterochromatic silencing is reinforced by ARID1‐mediated small RNA movement in Arabidopsis pollen. New Phytol. https://doi.org/10.1111/nph.16871 (2020)
Nurse cell–derived small RNAs define paternal epigenetic inheritance in Arabidopsis
Plants encode a general siRNA suppressor that is induced and suppressed by viruses
A plant germline-specific integrator of sperm specification and cell cycle progression
Artificial microRNAs reveal cell-specific differences in small RNA activity in pollen
Epigenetic reprogramming rewires transcription during the alternation of generations in Arabidopsis
Arabidopsis male sexual lineage exhibits more robust maintenance of CG methylation than somatic tissues
Pollen tetrad-based visual assay for meiotic recombination in Arabidopsis
Arabidopsis RNA polymerase IV generates 21–22 nucleotide small RNAs that can participate in RNA-directed DNA methylation and may regulate genes
Paternally acting canonical RNA-directed dna methylation pathway genes sensitize arabidopsis endosperm to paternal genome dosage
The Arabidopsis Mutant jason produces unreduced first division restitution male gametes through a parallel/fused spindle mechanism in meiosis II
An imprinted gene underlies postzygotic reproductive isolation in Arabidopsis thaliana
Hypomethylated pollen bypasses the interploidy hybridization barrier in Arabidopsis
Bypassing reproductive barriers in hybrid seeds using chemically induced epimutagenesis
Induction of RNA-directed DNA methylation upon decondensation of constitutive heterochromatin
Borg, M. et al. Targeted reprogramming of H3K27me3 resets epigenetic memory in plant paternal chromatin. Nat. Cell Biol. https://doi.org/10.1038/s41556-020-0515-y
Buttress, T. et al. Histone H2B.8 compacts flowering plant sperm through chromatin phase separation. Nature https://doi.org/10.1038/s41586-022-05386-6
Non-cell-autonomous small RNA silencing in Arabidopsis female gametes
Asymmetric expression of Argonautes in reproductive tissues
Herridge, R. P. et al. Pseudouridine guides germline small RNA transport and epigenetic inheritance. Preprint at https://doi.org/10.1101/2023.05.27.542553 (2023)
Floral dip: a simplified method for Agrobacterium -mediated transformation of Arabidopsis thaliana
Bismark: a flexible aligner and methylation caller for Bisulfite-Seq applications
Transgenerational effect of mutants in the RNA-directed DNA methylation pathway on the triploid block in Arabidopsis
Download references
This work was supported by the grant EpiHYBRIDS from the French National Agency of Research (ANR-19-CE120008 to F.B.)
We thank all members of the EPIREP team for daily discussions
Hervé Vaucheret for critical reading of the manuscript and sharing the p35S::RTL1-Myc plasmid and seeds
and Gregory Copenhaver for the FTL1230 line
The authors acknowledge technical support from Mickael Bourge and Nicolas Valentin from the cytometry facility of the I2BC
The IJPB benefits from the support of Saclay Plant Sciences-SPS (ANR-17-EUR-0007)
Present address: School of Biosciences and Technology
analyzed the data and wrote the manuscript with contributions from K.P
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DOI: https://doi.org/10.1038/s41467-024-48950-6
Two start-ups have launched to develop next-generation drugs using small interfering RNA (siRNA) to silence genes
is a spin-off of the venture capital firm Atlas Venture
The company spent about 3 years in stealth while designing a drug candidate that combines a ligand with siRNA that should silence messenger RNA (mRNA) and
reduce the number of certain solute carrier proteins that are involved in disease
While siRNA is a proven therapeutic approach
getting it to the right cell types is challenging
The kidney is a “very complex tissue,” says Chief Scientific Officer Alfica Sehgal
a former head scientist at RNA biotech firms Camp4 Therapeutics and Alnylam Pharmaceuticals
The organ consists of multiple tissue types
also filters out molecules by size; it excretes siRNA by default
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The company spent about 3 years in stealth while designing a drug candidate that combines a ligand with siRNAthat should silence messenger RNA (mRNA) and
“It’s not an easy bean to crack,” Sehgal says
But Judo Bio has proposed an elegant solution
The ligand acts as a hook on the siRNA so that
the conjugate latches on to the kidney’s proximal tubule epithelial cells via a receptor called megalin
The start-up recently closed a series A investment round that
While Judo Bio was preparing for its public launch
the latest project of Alnylam founding CEO John Maraganore
Maraganore is partial to RNA interference (RNAi) as a drug mechanism; in 2018
Alnylam became the first company to have an RNAi drug approved by the US Food and Drug Administration
So in the summer of 2023, when Maraganore came across a paper from chemist Kotaro Nakanishi at the Ohio State University, he was intrigued. Nakanishi and his colleagues had found that certain, tiny RNA molecules could activate protein argonaute-3 to slice through proteins (Proc. Natl. Acad. Sci. U.S.A. 2020, DOI: 10.1073/pnas.2015026117)
They called the molecules cleavage-inducing tiny guide RNAs
A seed was planted: use those minuscule RNAs to get to tissues that large molecules—like traditional siRNA—can’t reach
Maraganore sees potential for cityRNAs to help silence disease-causing genes in multiple target tissues
He expects City will start testing its first drug candidate in humans by early 2026 with the help of a $135 million series A financing round led by Arch Venture Partners
Maraganore envisions one to two clinical trials for new drug candidates beginning each year
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Copyright © 2025 American Chemical Society
Small interfering RNA (siRNA) carries great promise in the biotechnology industry
As an essential component of the RNA interference (RNAi) pathway
siRNA works by degrading target messenger RNA (mRNA) molecules
thereby preventing them from being translated into proteins
This specific mechanism has the potential to treat a wide range of diseases
from genetic disorders and cancers to viral infections.
which carries genetic information for protein synthesis
which regulates gene expression more broadly
siRNA is designed to target and silence specific genes with precision
According to Maximize Market Research
the market for siRNA therapeutics is expected to grow from $12.7 billion to $39.2 billion by 2029
Here are eight companies contributing to the field of siRNA
Founded in 2002 and headquartered in Cambridge, Massachusetts, Alnylam Pharmaceuticals is a leader in RNAi therapeutics
The company leverages its proprietary platforms
the enhanced stabilization chemistry (ESC) platform
and its conjugate delivery platform.
The ESC platform incorporates chemical modifications to the siRNA molecules
which enhance their stability and reduce the likelihood of degradation within the body
This allows for longer-lasting therapeutic effects and less frequent dosing
The conjugate delivery platform involves the use of GalNAc (N-acetylgalactosamine) conjugates
By attaching GalNAc ligands to siRNA molecules
Alnylam can deliver these therapeutics directly to hepatocytes (liver cells) with high precision
This targeted delivery system enhances the efficacy of the siRNA while minimizing off-target effects and potential toxicity
The biotech company is well-established in the siRNA field and has several commercialized products on the market:
Founded in 2017 and headquartered in Philadelphia
Aro Biotherapeutics specializes in developing tissue-targeted genetic medicines
The company’s proprietary Centyrin technology enables the precise delivery of therapeutic agents to specific cells
Aro’s Centyrin technology involves small
stable proteins that are engineered to bind specifically to disease targets
This technology is particularly effective for delivering siRNA to extra-hepatic tissues
Centyrin-siRNA conjugates allow for targeted delivery to tissues like muscle
where traditional siRNA therapies struggle to reach
This targeted approach enhances the efficacy and safety profile of siRNA therapies by minimizing off-target effects and ensuring that the therapeutic molecules reach the intended cells
is a Centyrin-siRNA conjugate targeting Pompe disease
inherited metabolic disorder caused by mutations in the GAA gene
This gene mutation leads to a deficiency of the enzyme acid alpha-glucosidase
which is crucial for breaking down glycogen into glucose
causing progressive damage to muscle and nerve cells throughout the body.
This therapy is currently in phase 1 clinical trials and has received both orphan drug designation and rare pediatric disease status from the FDA
ABX1100 works by targeting glycogen synthase 1 (Gys1) mRNA in muscle tissues
reducing the toxic glycogen buildup that characterizes Pompe disease
Aro Biotherapeutics has raised significant funding, with a recent $41.5 million series B financing round in November 2023. The company recently started its first-in-human clinical trial for ABX1100
Arrowhead Pharmaceuticals specializes in developing RNAi-based therapies
Arrowhead’s Targeted RNAi Molecule (TRiM) platform is designed to enable precise delivery of siRNA molecules to specific tissues
The TRiM platform optimizes siRNA stability
reducing off-target effects and improving therapeutic outcomes
allowing different chemical components to be swapped in and out to best suit the target and disease
Arrowhead collaborates with pharmaceutical giants like Takeda
and GSK to co-develop and commercialize RNAi therapies
The company focuses on developing RNAi-based therapies to address genetic and rare diseases
Dicerna’s GalXC RNAi technology employs a structure where siRNA molecules are chemically conjugated to a GalNAc ligand
This ligand targets receptors highly expressed in liver cells
ensuring the siRNA is efficiently delivered to the liver
where it can bind to and degrade the target mRNA
reducing the production of disease-causing proteins
The two key candidates that motivated Novo Nordisk to acquire the siRNA company in addition to its technology are Rivfloza and Belcesiran.
The FDA approved Rivfloza (nedosiran) for treating primary hyperoxaluria type 1 (PH1) in children 9 years and older and adults with relatively preserved kidney function
PH1 is an inherited disorder caused by a deficiency of the liver enzyme alanine-glyoxylate aminotransferase (AGT)
This enzyme deficiency leads to the overproduction of oxalate
a substance that combines with calcium to form insoluble calcium oxalate crystals
These crystals can accumulate in the kidneys and urinary tract
leading to kidney stones and progressive kidney damage
Rivfloza is a once-monthly subcutaneous therapy designed to lower urinary oxalate levels by targeting the liver enzyme lactate dehydrogenase
Belcesiran targets alpha-1 antitrypsin deficiency (AATD) by silencing the mutant gene responsible for the disease
AATD is a genetic disorder caused by mutations in the SERPINA1 gene
AATD primarily affects the liver and lungs
leading to conditions such as liver cirrhosis and emphysema
Prior to its acquisition, Dicerna secured a substantial total funding of $420.5 million
Dicerna’s technologies and pipeline have been integrated into Novo’s broader therapeutic programs
expanding the application of RNAi therapies
Founded in 2017, DTx Pharma is a biotechnology company that focuses on developing RNA-based therapies using its proprietary Fatty Acid Ligand Conjugated OligoNucleotide (FALCON) platform. In July 2023, Novartis acquired the siRNA company for an upfront payment of $500 million
with potential milestone payments bringing the total value up to $1 billion.
and potency of siRNA molecules by conjugating them with fatty acids
This modification improves the biodistribution and cellular uptake of siRNA
enabling efficient gene silencing in tissues beyond the liver
such as the central nervous system and muscles
This approach leverages the natural uptake mechanisms of cells for fatty acids
thereby “tricking” cells into absorbing the siRNA for targeted gene repression
with plans to start clinical trials in the near future
Founded in 2020 and with activities in the U.K.
this biotech company focuses on developing durable siRNA therapies through a combination of chemistry and artificial intelligence
Eleven Therapeutics employs its proprietary TERA platform
which integrates parallel combinatorial chemistry with AI algorithms to design and optimize RNA molecules
The platform uses a high-throughput split-pool synthesis process to generate a vast library of chemically modified RNA molecules
Each molecule is tagged with a DNA barcode
enabling precise tracking and analysis of its structure-activity relationship (SAR)
The process involves the following key steps:
Eleven Therapeutics raised $22 million in seed funding in 2022
including a substantial contribution from the Bill & Melinda Gates Foundation
The CASi platform combines properties of both single and double-stranded RNAs to enable efficient self-delivery
CASi molecules are designed to be activated only under specific cellular conditions
ensuring that the siRNA is delivered and activated only in target cells
This specificity reduces off-target effects and enhances the therapeutic index of the siRNA therapy
The siRNA company is initially focused on developing treatments for neurodegenerative diseases but also works on central nervous system diseases
The biotech’s siRNA programs are still at the preclinical stage
Wave Life Sciences was founded in 2012 and is headquartered in Cambridge
It is a clinical-stage biotechnology company focused on developing RNA-targeting therapeutics
The company’s proprietary PRISM platform integrates multiple RNA technologies
The company employs siRNA constructs enhanced with GalNAc conjugation
which improves targeted delivery to liver cells
This method leverages the natural uptake pathways of cells
enhancing the precision and effectiveness of siRNA therapies
The biotech’s INHBE program targets metabolic disorders, including obesity. Utilizing Wave’s GalNAc-siRNA technology, the INHBE program has shown promising preclinical results
including substantial weight loss and reduction in visceral fat in animal models
The program is expected to enter clinical trials in early 2025
Wave Life Sciences has a significant partnership with GSK, focusing on siRNA and RNA editing programs. GSK has selected two siRNA programs to advance to development candidates
utilizing Wave’s GalNAc-siRNA format for hepatology applications
The collaboration with GSK includes the development of up to eight RNA-targeting programs
with Wave leading the research up to the investigational new drug (IND) stage.
The field of siRNA therapeutics is poised for substantial growth
This rapid expansion is driven by advancements in RNAi technology
and the successful approval and commercialization of several siRNA-based drugs
Key players like Alnylam Pharmaceuticals have paved the way with FDA-approved therapies such as ONPATTRO or GIVLAARI
collaborations between biotech companies and pharmaceutical giants
such as the partnership between Wave Life Sciences and GSK
the field of siRNA therapeutics faces several challenges
One of the primary hurdles is the effective delivery of siRNA molecules to target cells
The hydrophilic and negatively charged nature of siRNA makes it difficult for these molecules to cross cell membranes and reach the cytoplasm
such as lipid nanoparticles (LNPs) and GalNAc conjugates
have been developed to enhance cellular uptake and target specificity
Another challenge is the potential for off-target effects and immune responses
Chemical modifications to the siRNA structure can help mitigate these issues
enhancing stability and reducing immunogenicity
Ongoing research is focused on refining these modifications and developing more sophisticated delivery systems to overcome these barriers
Oncology R&D trends and breakthrough innovations
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