He was a Veteran of the United States Army and then later served in the National Guard
Reverend Caldwell was a licensed minister with the South Carolina International Pentecostal Holiness Conference
member of Lake City Pentecostal Holiness Church
along with serving in various positions with the SCIPHC and serving as a supply Pastor for several churches in the area
of Lake City and Joshua Mark (Morgan) Caldwell of Odessa
Ester Bella Caldwell and Julia Caldwell; brother
Joy Moore of Fountain Inn; numerous nieces
Reverend Caldwell was preceded in death by his son
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Elizabeth Caldwell and Grace Caldwell; brothers
Curtis Woodrow Caldwell and Nealy Caldwell; sister
to follow at Camp Branch Pentecostal Holiness Church Cemetery
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Introduction: Bioproduction of plant-derived triterpenoids in recombinant microbes is receiving great attention to make these biologically active compounds industrially accessible as nutraceuticals, pharmaceutics, and cosmetic ingredients. So far, there is no direct method for detecting triterpenoids under physiological conditions on a cellular level, information yet highly relevant to rationalizing microbial engineering.
Methods: Here, we show in a proof-of-concept study, that triterpenoids can be detected and monitored in living yeast cells by combining coherent anti-Stokes Raman scattering (CARS) and second-harmonic-generation (SHG) microscopy techniques. We applied CARS and SHG microscopy measurements, and for comparison classical Nile Red staining, on immobilized and growing triterpenoid-producing, and non-producing reference Saccharomyces cerevisiae strains.
Results and Discussion: We found that the SHG signal in triterpenoid-producing strains is significantly higher than in a non-producing reference strain, correlating with lipophile content as determined by Nile red staining. In growing cultures, both CARS and SHG signals showed changes over time, enabling new insights into the dynamics of triterpenoid production and storage inside cells.
Volume 11 - 2023 | https://doi.org/10.3389/fbioe.2023.1106566
Introduction: Bioproduction of plant-derived triterpenoids in recombinant microbes is receiving great attention to make these biologically active compounds industrially accessible as nutraceuticals
there is no direct method for detecting triterpenoids under physiological conditions on a cellular level
information yet highly relevant to rationalizing microbial engineering
that triterpenoids can be detected and monitored in living yeast cells by combining coherent anti-Stokes Raman scattering (CARS) and second-harmonic-generation (SHG) microscopy techniques
We applied CARS and SHG microscopy measurements
and for comparison classical Nile Red staining
on immobilized and growing triterpenoid-producing
and non-producing reference Saccharomyces cerevisiae strains
Results and Discussion: We found that the SHG signal in triterpenoid-producing strains is significantly higher than in a non-producing reference strain
correlating with lipophile content as determined by Nile red staining
both CARS and SHG signals showed changes over time
enabling new insights into the dynamics of triterpenoid production and storage inside cells
the post-synthesis localization of triterpenoids is unclear
Schematic overview of the heterologous biosynthesis of lupane-type triterpenoids in S
The native yeast metabolism converts farnesyl pyrophosphate (FPP) to squalene (SQ) by squalene synthase (Erg9)
Squalene epoxidase (Erg1) catalyses the conversion of squalene to 2,3-oxidosqualene (OSQ)
The heterologous pathway constitutes an oxidosqualene cyclase (OSC)
catalyzing the cyclization of 2,3-oxidosqualene to lupeol
as well as a cytochrome P450 monooxygenase (CYP) and corresponding cytochrome P450 reductase (CPR)
Dashed arrows correspond to a hypothetical transfer of triterpenoids from the endoplasmic reticulum (ER) membrane into lipid droplets (LDs) and further to the plasma membrane
In addition to the unclear intracellular triterpenoid distribution between membranes and lipid droplets
there is little knowledge about triterpenoid production among individual cells of a population
Such insights would be valuable for understanding hydrophobic molecule trafficking and guiding strain engineering strategies
Due to the hydrophobic structure of triterpenoids
we assumed that Nile red staining is also a suitable method for detecting these compounds produced intracellularly by engineered yeast cells
We first applied Nile red staining to show that triterpenoid-producing strains differ from the reference strain regarding the accumulation of intracellular hydrophobic compounds
we tested the applicability of CARS and SHG microscopy to monitor triterpenoid accumulation in recombinant yeast
We performed CARS and SHG analyses for both fixed and live (growing) cells to evaluate the applicability of both methods for determining intracellular triterpenoid accumulation with temporal and spatial resolution
cerevisiae BA6∆ (unpublished) is a pah1 deletion mutant of BA6
generated through replacement of PAH1 with a hygromycin resistance cassette (YMR165C∆:hphMX)
Batch cultivations in 500 ml shake flasks started with a filling volume of 20 ml
A pre-culture was used to inoculate the main cultures to a start optical density measured at 600 nm (OD600) of 0.1
The optical density of the cultures was determined using a spectrophotometer (Ultrospec 10
Germany) with 0.5% phosphate-buffered saline (PBS) used as blank
A predetermined correlation factor of 0.29 g cell dry weight (CDW) per unit OD600 for strain BA6∆ and 0.2 for BA6 and the reference was used to derive the CDW concentration
The cultivations took place in a rotary shaker (New Brunswick Innova 44R) at 30°C
samples were taken during exponential growth on glucose and after the diauxic shift during growth on ethanol
For static, non-shaken cultivations, we designed the experimental setup shown in Figure 2
Experimental setup of static culture experiments
Static culture experiments took place in a glass-bottom microscopy chamber with a coverslip (ibidiplates μ-Slide 4 Well Glass Bottom
Three of the four chambers were filled with 1 ml of the yeast culture at a starting OD600 of 0.4
The chamber was fitted onto the microscope directly below the objective lens to take microscopy images of each chamber at regular intervals
The cultures were aerated with ambient air to prevent oxygen limitation
sterile air was moisturized with water and ethanol by passing it through an ethanol:water solution (50:50 (v/v))
Two holes on both ends of the lid served as gas inlet and outlet; a third opening in the dividing wall ensured gas exchange between the two chambers
Arrows indicate airflow through the chambers
Samples of 800 μL of culture broth were transferred into 2 ml sample tubes for the analysis of intracellular triterpenoid concentrations and stored at −20°C until further processing or immediately analyzed
Cells were disrupted by adding 250 μL of glass beads (smooth 500 μm
and 800 μl chloroform:methanol (ratio 80:20
v/v) and vigorously agitating in the Mini-Beadbeater 16 (BioSpec Products
Samples were centrifuged for 10 min at 13,000 rpm (16,089 x g) and 5°C
200 μl of the lower organic phase were transferred into a glass vial (VVial
Phenomenex) containing an insert (15 mm tip
KG Germany) for High-Performance Liquid Chromatography (HPLC) analysis
Product quantification was conducted with a reverse HPLC system (Thermo Fisher UltiMate 3,000 Dionex)
Samples were kept a 4°C in an autosampler (Thermo Fisher UltiMate 3,000)
Five µL of the sample were injected into a C18 column (Merck Spherisorb ODS-2 (5 μm)
Germany) with a guard column (EC 4/3 NUCLEODUR C18 Gravity
while the column temperature was kept at 40°C in a thermostatic column compartment (Thermo Fisher UltiMate 3,000)
Analytes were eluted using gradient chromatography at 1.2 mL/min flow rate using a binary pump (Ultimate 3,000 Pump
Solvent B was 0.2% (v/v) formic acid of high purity (≥98%)
The linear gradient method was as follows: 20% B from 0 to 1 min
then back to 20% B from 23 to 26 min
Solvents were degassed using an online degasser
Analytes of interest were monitored using a charged aerosol detector (CAD
esa ERC GmbH) driven by a nitrogen generation system (Parker
two times 800 μl were taken from the same cultivation
serial dilutions (df = 2) of standards for lupeol (Sigma Aldrich
and betulin aldehyde (Cfm Oskar Tropitzsch GmbH
Yeast cells were immobilized on agarose beds for microscopic analyses
One ml of warm 1% agarose gel was applied onto a microscope slide and covered with a second microscopy slide to force the formation of a planar surface
Ten µL of a culture diluted to an OD600 of 1.0 was applied on the agarose layer and protected with a cover glass
Desiccation of samples was prevented by covering the edges of the coverslip with clear lacquer and analyzing samples immediately
Nile Red staining was performed based on a protocol described in Zuriani et al. (2013)
was centrifuged at 12,000 g for 5 min
and the pellet was resuspended in 1 mL 0.5% PBS
60 μl of Nile red (80 μg/mL dissolved in acetone) was added to the cell suspension
The samples were incubated for 30 min at RT in the dark
samples were centrifuged again at 12,000 g for 5 min
Pellets were carefully resuspended in 1 mL 0.5% PBS
and 100 μl of the sample were transferred to a 96-well microplate
Fluorescence was measured at different excitation (Ex) and emission (Em) wavelengths using the Multi-Mode Microplate Reader Synergy; Ex/Em 550/638 nm for phospholipids
23°C) with the following parameters: read height 8 mm
≥95%) were analyzed in crystalline conditions and squalene in liquid form
Saturated solutions of ergosterol and the main triterpenoid products
betulin and betulinic acid in ethanol were prepared to analyze the CARS and SHG spectra in their dissolved state
Assuming additivity of the signal intensities
the mean intensities of dissolved substances were corrected by subtracting the mean CARS signal intensity of pure ethanol
The difference in mean intensities is the estimated CARS signal caused by these substances
While betulin and betulinic acid generated only a weak CARS signal
ergosterol produced a stronger CARS signal in solution
We also determined the number of SHG pixels not colocalizing with CARS. The term was normalized for each object using Eq. 3 by dividing with the total object pixel size
The total object pixel size refers to the total pixels
independent of the threshold of 25% of the maximum intensity
The altered lipophilic molecule profiles (lipids
triterpenoids) make these strains excellent test objects for evaluating techniques for analyzing the intracellular compositions in yeast
We used this stain to confirm differences in the hydrophobic compound composition of the chosen yeast strains
a prerequisite for CARS and SHG measurements
We measured the fluorescence at two different excitation and emission wavelengths: Ex/Em 515/583 nm for neutral lipids and 550/638 nm to detect polar phospholipids
Since this method falls short of distinguishing the different heterologous and native lipophilic compounds
more definitive explanations cannot be given
Qualitative determination of the hydrophobic molecule content of engineered yeast
B): Fluorescence intensity [-] at Ex/Em 515/583 nm (A)
550/638 nm (B) of Nile red-stained cell suspensions of the reference strain (Ref)
and the two betulinic acid-producing strains BA6 and BA6∆ sampled from a batch cultivation during growth on glucose (I) and after the diauxic shift during growth on ethanol (II)
The OD600 of all samples was adjusted to 1
(C) Triterpenoid yield [mg/gCDW] of the reference strain (Ref) and the two betulinic acid-producing strains BA6 and BA6∆ sampled from a batch cultivation during growth on glucose (I) and after the diauxic shift during growth on ethanol (II)
Nile red staining indicated compositional differences between the reference and triterpenoid-producing yeast strains
Single-cell microscopy imaging techniques are required for subcellular localization of triterpenoids or time-resolved tracking of triterpenoid distribution in individual cells and molecule partitioning during cell proliferation
we tested the applicability of CARS and SHG microscopy techniques as non-invasive methods for analyzing living yeast cells
we analyzed pure standards of triterpenoids and ergosterol to observe their detectability by CARS and SHG techniques
Ergosterol was included to estimate interference with triterpenoid signals because of its structural and biophysical similarity and the differential accumulation in the tested yeast strains
Evaluating CARS and SHG measurements for triterpenoid detection
and an overlay of both signals of solid ergosterol
Solid compounds were measured in xy and liquid squalene in xz dimension
Yellow areas in the overlay images emerge through colocalization of CARS and SHG signals
green or red are areas with solely or predominantly SHG or CARS signal
respectively; edge length = 75 µm
Likewise, ethanolic solutions of ergosterol, betulin, and betulinic acid showed a CARS signal but no SH activity (Figure 5)
Transmission microscopy showing laser reflection (T) (white)
and SHG (green) signals of pure ethanol and solutions of ergosterol
and betulinic acid in ethanol at 817 nm
edge length = 75 µm
total triterpenoids (sum of betulinic acid
and triterpenoid content of the investigated strains during growth in batch culture on glucose (I) and after the diauxic shift on ethanol (II)
CARS and SHG measurements of triterpenoids in yeast
and the overlay of CARS and SHG signals for the reference (Ref) and triterpenoid producing strains BA6 and BA6∆ at early (I) and late fermentation stage (II)
Measurements were performed at 816 nm; edge length is 25 µm
the SHG signal in the reference strain was noticeably lower than in the triterpenoid-producing strains
Together with the SHG signal of solid triterpenoid standards
the SH activity of BA6 and BA6∆ cells suggests that it is caused by triterpenoid agglomerates or (pseudo) crystals
BA6∆ cells showed cell-to-cell heterogeneity in SHG, especially during stage I. Similarly, previous studies reported variability in endoplasmic reticulum morphology and lipid droplet abundance between single BA6∆ cells (Walter, 2018)
which might therefore differ in lipid composition
if the here observed variability in SHG signal relates to this phenotype or differences in triterpenoid accumulation or lipid content cannot be stated
Immobilized cells of the reference and engineered strains sampled during stage II showed comparable CARS signals. Spherical structures were detected by CARS in all three strains (Figure 6)
the SHG signal in triterpenoid-producing strains was much higher than in the non-producing strain
The overlay of the CARS and SHG signals allows speculation of analyte distribution
While most regions show a colocalization (indicated by the yellow color)
there are also regions with only or predominantly SHG or CARS activity
areas of presumed lipid droplet localizations showed no SHG signal
suggesting that triterpenoids are either not present in these organelles or are not in a crystal-like form required for exerting SH activity
regions with a predominant SH signal suggest the agglomeration of solid triterpenoid particles in a low-lipid environment
The overlay of CARS and SHG of solid sterols/terpenoids shows a predominance of SHG at least for some compounds
Hence pixels with SHG non-colocalized with CARS point to the enrichment of these molecules in solid/pseudocrystal form and in a low-lipid environment
when located in lipid membranes and lipid droplets
always result in both CARS and SHG signals
our results hypothesize that triterpenoids might also accumulate in other cellular spaces or be enriched in microdomains (lipid raft-like structures) within membranes
Box plot representation of colocalization analysis for the reference (Ref) and triterpenoid producing strains BA6 and BA6∆ during growth stage I and II
(A): Ratio of SHG/CARS signal colocalization
(B): Ratio of CARS signal colocalizing with SHG signal
(C): Ratio of SHG signal not colocalizing with CARS normalized to the total object pixel size
Dots outside the box: Outliers; Vertical lines: Whiskers; Dots inside the box: Means; Horizontal line inside the box: median
The colocalization analysis was performed for single objects (representing single cells and in some cases cell agglomerates) in the microscopy image of each strain
The number of cells per image for the different strains was as follows: BA6 (I)
The large variance in some data sets indicated by the whiskers and outliers may have been caused by biological heterogeneity between individual cells and analytical challenges when cell agglomerates are formed
these results indicate a correlation of SHG signal with triterpenoid accumulation and the subcellular distribution
Overall and important for the scope of this study
The potentially higher ergosterol content could also have contributed to the higher SHG signal excreted by cells under these growth conditions compared to cells from glucose batch cultivations
Time resolved triterpenoid production in yeast
Measurement of CARS (red) and SHG (green) signals and the overlay for the reference strain (Ref)
and triterpenoid producing strains BA6 and BA6∆ during growth on ethanol in a static-culture
Overlay images show yellow in areas of strong colocalization of CARS and SHG
Cultivation took place at room temperature
The culture was aerated with a water and ethanol solution (50:50 v/v)
Measurements were performed at 816 nm; edge length = 25 µm
Also, considerable differences in the CARS and SHG signals were observed throughout the cultivation of the triterpenoid-producing strains BA6 and BA6∆. The SHG signal increased in both cultures over time, indicating accumulation of triterpenoids. While the SHG signal in BA6 was nearly equal in all cells, for BA6∆, some differences were observed in the SHG signal of individual cells. Figure 8 shows 3 cells of BA6∆ that form a cluster
The larger size of the upper cell suggests it to be an old cell
explaining its high SHG signal from the beginning
the two smaller cells had a weak SHG signal at the beginning
likely correlating with intracellular triterpenoid accumulation
The overlay of SHG and CARS pictures revealed no or very few colocalizations
indicating that the triterpenoids were mostly not present in soluble form in a lipid rich environment
Whether they are locally enriched in lipid membranes or even present in an aqueous surrounding
the vacuole cannot be distinguished with the current measurements
One limitation of the here presented methodology is that CARS also detects triterpenoids (Yu et al., 2008)
the signals of both methods should be considered for a deeper evaluation of the results
These data show clear differences in producing and non-producing strains and importantly allow time-resolved observation on single cell level—the greatest advantages of the applied non-invasive microscopy technique compared to analytical methods
which provide an averaged triterpenoid concentration of an entire population
we used three techniques (Nile red staining
CARS and SHG microscopy) to analyze lipid compounds and triterpenoids in yeast cells
We could show that the combination of the non-invasive techniques CARS and SHG allow detection of lipids and triterpenoids in living yeast cells
This highlights the great potential of these methods for future analysis of natural product synthesis with special and temporal resolution
Other than conventional methods like Nile red
the application of CARS and SHG allows the detection of both triterpenoids and lipids in individual cells
The application of CARS and SHG signal measurement shows potential for further development and an advanced quantification
detection of the individual triterpenoid components at different wavelengths would be an option to further improve the existing method towards more specific and quantitative analysis
Using the current state-of-the art techniques
we were able to monitor triterpenoid accumulation in cells of a population over the entire cultivation time
this is the first time that the combination of both CARS and SHG techniques are applied for the analysis of intracellular product accumulation in living yeast cells
This proof-of-principle study shows the potential of application of CARS and SHG microscopy techniques in applied microbiology allowing new insights into the dynamics of triterpenoid production and storage by recombinant yeasts
The raw data supporting the conclusion of this article will be made available by the authors
and MD conceptualized and designed of the study
All authors contributed to manuscript revision
This research was performed within the project PRODIGY (process-directed drug generation in yeast) funded by the German Federal Ministry of Education and Research BMBF (grant No
We would like to share our gratitude to our project partners Prof
Markus Nett and Anna Tippelt (Department of Biochemical and Chemical Engineering
TU Dortmund University) for their support and enabling us to perform our yeast cultivations in their laboratory
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
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
The Supplementary Material for this article can be found online at: https://www.frontiersin.org/articles/10.3389/fbioe.2023.1106566/full#supplementary-material
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Freier E and Ebert BE (2023) Non-invasive monitoring of microbial triterpenoid production using nonlinear microscopy techniques
Received: 23 November 2022; Accepted: 23 January 2023;Published: 28 February 2023
Copyright © 2023 Dianat, Münchberg, Blank, Freier and Ebert. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use
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provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited
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*Correspondence: Birgitta E. Ebert, YmlyZ2l0dGEuZWJlcnRAdXEuZWR1LmF1; Erik Freier, ZXJpay5mcmVpZXJAdW5pLXd1cHBlcnRhbC5kZQ==; Lars M. Blank, bGFycy5ibGFua0Byd3RoLWFhY2hlbi5kZQ==
†ORCID: Mariam Dianat, orcid.org/0000-0001-6430-6146; Lars M. Blank, orcid.org/0000-0003-0961-4976; Erik Freier, orcid.org/0000-0002-0559-4210; Birgitta E. Ebert, orcid.org/0000-0001-9425-7509
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Metrics details
Redox-active films were proposed as protective matrices for preventing oxidative deactivation of oxygen-sensitive catalysts such as hydrogenases for their use in fuel cells
the theoretical models predict quasi-infinite protection from oxygen and the aerobic half-life for hydrogenase-catalyzed hydrogen oxidation within redox films lasts only about a day
we employ operando confocal microscopy to elucidate the deactivation processes
The hydrogen peroxide generated from incomplete reduction of oxygen induces the decomposition of the redox matrix rather than deactivation of the biocatalyst
We show that efficient dismutation of hydrogen peroxide by iodide extends the aerobic half-life of the catalytic film containing an oxygen-sensitive [NiFe] hydrogenase to over one week
approaching the experimental anaerobic half-life
our data support the theory that redox films make the hydrogenases immune against the direct deactivation by oxygen and highlight the importance of suppressing hydrogen peroxide production in order to reach complete protection from oxidative stress
a Structure of the [NiFe]-hydrogenase and the viologen-modified polymer (polyethylenimine backbone)
b Proposed mechanism for protection from O2
The hydrogenase catalyzes the reversible oxidation of H2 in the inner parts of the film and generates electrons that are transferred to the electrode via the viologen (Vred/Vox) moieties (pathway 1) which produces the catalytic current when an oxidative potential is applied to the electrode
the presence of O2 in the electrolyte creates an oxidative driving force that diverts some of the electrons towards the electrolyte/film interface (pathway 2) where the viologen moieties act as catalysts for O2 reduction
thus protecting the catalyst in the inner film domain but also producing H2O2
Iodide catalyzes the subsequent H2O2 dismutation to H2O and half a molecule of O2
and demonstrate that suppression of reactive oxygen species is also necessary to avoid oxidative degradation of the catalytic films
While dismutation of two molecules of H2O2 generates one molecule of O2
successive cycles of the viologen-catalyzed O2 reduction reaction and of the iodide-catalyzed H2O2 decomposition results in H2O as the sole end product
3 mm in diameter) were coated with viologen-modified polymer with a surface coverage of 2.2 mg cm−2
pH 7) with 10 µL stock solution of Amplite™ Fluorimetric Hydrogen Peroxide Assay Kit
The fluorescence of the oxidized viologen-modified films was collected around its maximum emission of 590 nm upon excitation at 488 nm
The emission of the H2O2 fluorescent probe was determined around its maximum emission of 660 nm upon excitation at 633 nm
All measurements were performed under ambient air and at 300 K
This demonstrates that O2 reduction catalyzed by the viologen-modified film generates H2O2
and that H2O2 can be efficiently dismutated when iodide is present in the electrolyte
Error bars are defined as standard deviation
Average values and standard deviations were obtained from measurements at three individually prepared electrodes and then normalized by average ip values before O2 reduction
All measurements were performed with GCE (3 mm in diameter) coated with viologen-modified polymer with a surface coverage of 0.3 mg cm−2
Source data are provided as a Source Data file
the conclusion from the CV results is that loss of viologen peak current is associated with H2O2 generation
These observations highlight the need for efficient dismutation of H2O2 generated from the viologen-catalyzed O2 reduction reaction in order to avoid decomposition of the redox hydrogel film
The polymer surface coverage for all hydrogenase modified electrodes is 2.26 mg cm−2
complete reduction of O2 to water is necessary to bypass additional deactivation pathways involving reactive oxygen species that degrade the redox film
the use of iodide is particularly advantageous since the dismutation of H2O2 leads to water and half a molecule of O2 that is further reduced by the viologen
and thus eventually leads to water as the sole final product
The iodide being used as a catalyst in this reaction is not used up and therefore represents a practical solution for long-term operation of energy converting systems in which H2O2 production is often an undesired side reaction of the system
This approach for H2O2 removal being exclusively based on tuning the composition of the electrolyte
rather than tuning the catalytic system itself
is directly applicable for enhancing the stability of other low potential electrochemical or photochemical systems suffering from degradation induced by H2O2 generation
an aqueous suspension of the viologen-modified polymer (4 µL
40 mg ml−1) and [NiFe] hydrogenase from Desulfovibrio vulgaris Miyazaki F (3 µL
pH 6.8) were mixed and applied to the GCE (3 mm diameter)
the polymer was drop-cast onto the GCE with surface coverages indicated in the captions of the figures
Tris buffer was added to the solution droplet (1 µL
pH 9) immediately after drop-casting to accelerate the polymer cross-linking via disulfide bond formation
Electrodes were stored at 4 °C in a closed vessel overnight
After 12 h the solution became turbid and was then left to dry in air for another hour before the electrochemical measurements
Fluorescence measurements were performed on a Leica Microsystems TCS SP8 CARS laser scanning microscope in a fully confocal optical setup
An argon gas laser excited the samples at 488 nm and an He–Ne laser was used for excitations at 633 nm
through an HC PL Fluotar ×10/0.3 dry or Fluotar VISIR ×25/0.95 water objective
The emission was detected in EPI direction with photomultiplier tubes (PMTs) from 500 to 630 nm
During fluorescence measurements the temperature in the sample compartment was stabilized at 300 K
The stock solutions of Amplite™ fluorimetric hydrogen peroxide assay kit were prepared according to the manufacturer’s protocol
CARS measurements were performed on a Leica Microsystems TCS SP8 CARS laser scanning microscope
A picoEmerald laser system from APE Berlin generated two synchronized pulsed laser beams at 817 and 1064 nm
which were temporally and spatially overlapped at the measurement position on the sample
The resulting CARS signal at 663 nm was detected via a non-descanned PMT
This corresponds to a Raman intensity at 2841 cm−1
The detection window of the PMT ranges from 560 to 750 nm
During CARS measurements the temperature in the sample compartment was stabilized at 300 K
The CARS lasers and signal detection were focused and collected via the same objectives as for the fluorescence measurements
The measurements followed each other in close succession (very few seconds)
All electrochemical measurements were carried out with BA Metrohm Autolab as well as a rotating-disc electrode setup
and O2 were controlled with mass-flow controllers
The reference electrode was Ag/AgCl/3 M KCl
Potentials are converted to the SHE using the correction ESHE = EAg/AgCl + 210 mV
All electrochemical measurements were performed at 298 K
the O2 concentration was monitored with FireStingGO2
Power curves were calculated from the steady-state currents obtained from stepped potential chronoamperometric experiments
A redox hydrogel protects hydrogenase from high-potential deactivation and oxygen damage
A redox hydrogel protects the O2-sensitive FeFe-hydrogenase from Chlamydomonas reinhardtii from oxidative damage
Mechanism of protection of catalysts supported in redox hydrogel films
Preventing the coffee-ring effect and aggregate sedimentation by in situ gelation of monodisperse materials
Heterogeneous ammonia and hydrogen production by MoFe protein
High-power formate/dioxygen biofuel cell based on mediated electron transfer type bioelectrocatalysis
Engineered electron-transfer chain in photosystem 1 based photocathodes outperforms electron-transfer rates in natural photosynthesis
Rational wiring of photosystem II to hierarchical indium tin oxide electrodes using redox polymers
Wiring of photosystem I and hydrogenase on an electrode for photoelectrochemical H2 production by using redox polymers for relatively positive onset potential
Cytochrome c-coupled photosystem I and photosystem II (PSI/PSII) photo-bioelectrochemical cells
Photosystem I (PSI)/Photosystem II (PSII)-based photo-bioelectrochemical cells revealing directional generation of photocurrents
A poly(cobaloxime)/carbon nanotube electrode: freestanding buckypaper with polymer-enhanced H2-evolution performance
Dual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen
Polymer-bound DuBois-type molecular H2 oxidation Ni catalysts are protected by redox polymer matrices
The oxidative inactivation of FeFe hydrogenase reveals the flexibility of the H-cluster
Oxygen-tolerant proton reduction catalysis
Dynamics of electron hopping in assemblies of redox centers
Rational design of quinones for high power density biofuel cells
A convenient electrochemical preparation of reduced methyl viologen and a kinetic study of the reaction with oxygen using an anaerobic stopped-flow apparatus
Impact of oxygen on glucose oxidation kinetics in a redox polymer mediated glucose oxidase electrode
On the parameters affecting the characteristics of the “wired” glucose oxidase anode
Oxygen reduction on redox mediators may affect glucose biosensors based on “wired” enzymes
How the reduction of O2 on enzymes and/or redox mediators affects the calibration curve of “wired” glucose oxidase and glucose dehydrogenase biosensors
Complete protection of O2-sensitive catalysts in thin films
Use of ‘split waves’ for the measurement of electrocatalytic kinetics
Methyl viologen mediated oxygen reduction on a boron-doped diamond electrode
The catalytic decomposition of hydrogen peroxide by the iodine-iodide couple at 25°
The iodide-catalyzed decomposition of hydrogen peroxide
Mechanistic details of an old reaction as revealed by electrospray ionization mass spectrometry monitoring
Cyclic voltammetry of electrocatalytic films: fast catalysis regimes
Cyclic voltammetry analysis of electrocatalytic films
Enhancing the biocompatibility and biodegradability of linear poly(ethylene imine) through controlled oxidation
Theoretical treatment of diffusion and kinetics in amperometric immobilized enzyme electrodes Part I
Spectroelectrochemical Characterization of the [NiFe] Hydrogenase of Miyazaki F
Properties of Purified Hydrogenase from the Particulate Fraction of Desulfovibrio vulgaris
Diazonium functionalisation of carbon nanotubes for specific orientation of multicopper oxidases: controlling electron entry points and oxygen diffusion to the enzyme
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Tobias Vöpel for discussions about the H2O2 reporter
Steffen Hardt for help with the fuel cell experiments
and Nina Breuer for the preparation of the DvMF [NiFe] hydrogenase
funded by the Deutsche Forschungsgemeinschaft (DFG
German Research Foundation) under Germany ́s Excellence Strategy—EXC-2033—Projektnummer 390677874
by the ERC starting grant 715900 and by the ANR-DFG project SHIELDS (PL 746/2-1)
is grateful for the support by the China Scholarship Council (CSC)
acknowledge funding by the “Ministerium für Kultur und Wissenschaft des Landes Nordrhein-Westfalen”
the “Regierender Bürgermeister von Berlin-inkl
and the “Bundesministerium für Bildung und Forschung”
also in the form of the Leibniz-Research-Cluster (grant number: 031A360E)
Leibniz-Institut für Analytische Wissenschaften – ISAS – e.V
Max-Planck-Institut für Chemische Energiekonversion
H.L performed all electrochemical experiments involving mediated electron transfer and contributed to the confocal fluorescence experiments
A.A.O contributed with direct electron transfer electrodes
performed the electrochemical modeling and simulations
conceived and performed the spectroscopic experiments
All authors contributed to writing the manuscript
The authors declare no competing interests
Peer review information Nature Communications thanks the anonymous 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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DOI: https://doi.org/10.1038/s41467-020-14673-7
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Medical/Hygiene
a leading manufacturer of wood-based cellulosic specialty fibres
and Hof University opened their new Nonwoven Development Center (VEZ)
Lenzing has access to a state-of-the-art development line at the campus in Münchberg with immediate effect
This offers new opportunities for sustainable fibre and nonwoven innovations for a wide range of applications including hygiene
In line with its sCore TEN corporate strategy
the Lenzing Group is focusing on sustainable innovations
which are agreed in an optimum manner to the needs of the value chain
“We offer our customers and partners a decisive competitive advantage - agility
The pilot plant in the VEZ allows the resource-efficient development of fibre and nonwoven innovations on a small scale”
Vice President Business Unit Nonwovens at Lenzing
The VEZ was completed according to schedule in September 2020
after Lenzing and the University of Hof signed a cooperation agreement for its use in 2019
such as the directive (EU) 2019/904 of the European Parliament and of the Council of 5 June 2019 on the reduction of the impact of certain plastic products on the environment
increase demand for responsibly manufactured nonwovens
The so-called Single-Use Plastics Directive aims at building awareness and greater transparency with regard to wet wipes and feminine hygiene products
With its Veocel branded wood-based cellulose fibres
Lenzing has been laying the foundation for many years for sustainable nonwoven applications and will test and develop innovative ideas using the new possibilities offered by the VEZ
“We are noticing increasing interest in sustainable concepts from biodegradable cellulose fibres”
Jürgen Eizinger sums up the market development of the last months and adds: “We are aware that the fibres used have an enormous influence on the final product
our commitment extends beyond fibre production.”
Lenzing will support customers and partners more intensively in the development of new nonwoven applications and at the same time promote cooperation in the field of marketing
the company already established new certification standards for the Veocel brand
Since then certified manufacturers can only use the Veocel logo with blends of biodegradable cellulosic fibres
the Veocel brand allows consumers to make a more conscious product selection
With its #ItsInOurHands environmental initiative
the Veocel brand also actively contributes to creating awareness
More detailed information can be obtained on itsinourhands.com
www.lenzing.com
Lenzing opens Center of Excellence in Indonesia
Lenzing applies for 25 patents for Lenzing Web Technology
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son of Thomas Keith Caldwell and Joy Munchberg Caldwell. He was a graduate of Williston-Elko High School
Reverend Caldwell was a member of Lake City Pentecostal Holiness Church
recently received his Ministerial Credentials and was an Honorary Discipleship Ministries Council Member with the South Carolina Conference IPHC
Inc. He was an avid Clemson fan and Carolina Panthers fan.
Tom Caldwell and Joy Caldwell of Turbeville; brothers
of Turbeville and Joshua (Morgan) Caldwell of Conway; nephews
Reverend Caldwell was preceded in death by his sisters Elizabeth Caldwell and Grace Caldwell; paternal grandmother
The family will receive friends from 3:00 – 4:00 PM
The two bestseller “Why Doesn’t Anyone Blush Anymore?” by Rabbi Manis Friedman and “The Book of Purpose” by Rabbi Tzvi Freeman have now been published in German by Books&Bagels in Switzerland
in German “Wird denn niemand mehr rot?” and “Das Buch vom Sinn”
were designed by the renowned book designer professor Ralf de Jong
easily understood and entertaining language how modesty can become a powerful tool for meaningful and intimate relationships
The publication of this book was made possible by the help of Bettina and Lutz Münchberg
“Das Buch vom Sinn” by Rabbi Freeman contains his condensed and sometimes directly quoted thoughts of the Rebbe about how to find purpose in life. It deals with questions about who we are, if our existence is an end to itself or if we can fill our lives with purpose and meaning. This book was published with the support of chabad.org
More information on the books can be found here: www.booksnbagels.com/liebe and here: www.booksnbagels.com/sinn
Supporting a well-founded textile-specific education in the new institute
Sandler AG has donated a professorship worth a total of EUR 600,000
Transport/Aerospace
a new textile research centre was inaugurated at Hof University’s Münchberg campus
together with other entrepreneurs and industry associations
has been decisively advocating the establishment of a textile research centre at Hof University’s Münchberg facility
the Bavarian state government approved the establishment of the institute
thus laying the foundation for the expansion of textile-specific education
which is deemed essential for Sandler and other companies in the region
it was a cause and at the same time a responsibility to further promote this field of education
Sandler decided to provide EUR 600,000 for an endowed professorship
The company thereby further contributes to the educational infrastructure in the region,” Sandler said
The new professorship has been filled since 2019 - Prof
Claus-Ekkehard Koukal holds a lectureship at the University of Applied Sciences Hof in the field of Innovative Textiles
teaching in the areas of nonwoven production
including the textile industry and research and development
he continues to be active in consultancy and research
The research project EFRE: The Future – Textile Industry 4.0
which focusses on the transfer of know-how from research to small and medium-sized companies; or the Traveltex project
which involves the development of functional knitted fabrics for travel clothing
“The close cooperation with universities and research centres is very important to us
we have been cultivating these partnerships for many years," explains Dr
"We are happy to be able to continue supporting textile-specific education in the region."
www.sandler.de
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Joy Buck of Northville is a fan of garage sales
the one-time shop owner often headed to the Upper Peninsula sightseeing with visitors
“Many friends and family came to visit,” she wrote in an email to the column
“My sister and her husband came to see us one time and our husbands went to the Sault to gamble at the casino.” While they did that
she and her sister would sometimes head out on the garage sale trail
she told appraiser Brian Thomczek at a recent Trash or Treasure day held at Judy Frankel Antiques
Buck came across a painting she had taken with her on two moves since
Titled “Pheasants,” it has a registration number of 19868 and is signed by “Majewicz,” she told the appraiser
“I have researched his work and feel that this may have value,” she continued
or if it really has any,” she told the appraiser
“I could never really find out more information about what it’s worth
The back of the oil on canvas is marked “G
Majewicz” and it is signed in the lower right
It measures 211/2 by 25 and features three pheasants in a landscape
Buck said that she found out a little more about the artist
and that while her information showed he was born in Germany
he was Polish and his forte was birds and wildlife
Internet research revealed a variety of wildlife and bird images by artist George Majewicz
The website askart.com list the artist’s birth date as 1897 and place as Polkowice/Munchberg and that he died in 1965
moreover especially in hunting and animal painting
He derives his motives mostly from the African animal world and devoted himself preferably to the representation of animals in the wilderness in connection with an impressive landscape description.”
Thomczek said the work could use a bit of restoration and cleaning and recommended former DIA employee Ken Katz
who runs the downtown’s Conservation and Museum Services (conservationandmuseumservices.com)
He told Buck that the frame alone is worth $150-$200; with the painting he’d appraise it at $300-$500
adding “that could go up if we had time to do more research on the artist and his sales records.”
he told her that she has a good eye and she should continue her garage sale hobby
It’s nicely done and definitely by a well-trained hand
Landscape scenes are popular paintings and it would be something that collectors
Do you have an object you would like to know more about
Send a photo and description that includes how you acquired the object to: The Detroit News
Include your name and daytime telephone number
You may also send your photo and description to trashortreas@aol.com
If chosen you’ll need to bring the items to an appraisal session
Polish death metal act Hate are in mourning after the death of their bassist Slawek 'Mortifer' Archangielskij
The musician passed away near the German town of Munchberg on the night of April 5 while the band was en route to their next gig on their European tour
Hate, who had been on the road in support of their latest album, 'Solarflesh,' posted about the loss of their comrade and stated that they'll immediately stop their current tour as a result of his death. Archangielskij was also the bass player for Naumachia and the guitarist for Saltus. Both of those bands reposted Hate's original Facebook message on his passing on their sites as well
The posting on the bassist's death reads as follows:
SŁAWEK „MORTIFER” ARCHANGIELSKIJ IS DEAD
At night 5th/6th April near a German town of Munchberg
best comrade and longtime bass player unexpectedly passed away
After the show in Stuttgart last night he went to sleep and never woke up
We found him lifeless early in the morning and immediately called an ambulance
Results of Sławek’s autopsy should be known soon
we decided to cancel the remaining shows and return home
We gave detailed testimonies to the German police
We are shocked and shattered by his sudden
We mourn together with Slawek’s family and friends
The death metal act has been around since 1990
but has gone through a number of bassists since their start
Archangielskij had been a touring member since 2007 and an official band member since 2009
Frontman Adam "ATF Sinner" Buszko remains the band's only original member
'Solarflesh' is Hate's eighth studio album
Watch the video for 'Alchemy of Blood' from Hate's 'Solarflesh' album below:
Polish death metal act Hate are in mourning after the death of their bassist Slawek 'Mortifer' Archangielskij. The musician passed away near the German town of Munchberg on the night of April 5 while the band was en route to their next gig on their European tour.\nRead More
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Shock in Split: Gennaro Gattuso set to leave Hajduk after Dinamo defeat
has set off on the adventure of a lifetime by deciding to walk to the Euro in Germany
with Detić planning to cover 40-50 km each day
with the use of public transport considered only in the case of serious injury
Detić will walk during the day and rest at night in a tent
and he hopes to receive support from fellow Croatians in the cities along the way
The thousand-kilometer journey began from Črešnjevo
Detić's ambitious trek aims to show his passion for football and his determination to support his team at the European Championship
Nogomania.com is a premier destination for football enthusiasts
delivering fresh and in-depth content from the heart of the Ex-Yu region's football scene.