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| Open AccessAn exposome atlas of serum reveals the risk of chronic diseases in the Chinese population
Current studies have provided limited knowledge on real-world chemical exposures and related risks. Here, the authors show serum exposure characteristics of humans in different regions and age groups, revealing diverse risk relationships with multiple chronic diseases.
- Lei You
- , Jing Kou
- & Guowang Xu
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Article
| Open AccessAutomating data analysis for hydrogen/deuterium exchange mass spectrometry using data-independent acquisition methodology
Manual data mining for HDX-MS restricts the use of this biophysical technique to a small number of samples run by specialty labs. Enabled by data-independent acquisition methodology, the authors describe an approach that fully automates and standardizes the information extraction process, opening the door to new and challenging applications.
- Frantisek Filandr
- , Vladimir Sarpe
- & David C. Schriemer
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Article
| Open AccessNanopore analysis of salvianolic acids in herbal medicines
Natural herbs, which contain pharmacologically active compounds, have been historically used as medicines but the analysis of their chemical components is time-consuming and complex. Here, the authors report a phenylboronic acid appended Mycobacterium smegmatis porin A (MspA) nanopore for sensing a variety of bioactive compounds based on salvianolic acid, without the need for sample separation or purification.
- Pingping Fan
- , Shanyu Zhang
- & Shuo Huang
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Article
| Open AccessNanopore analysis of cis-diols in fruits
Fruits contain a large variety of cis-diols but their rapid and direct analysis without complex sample pretreatment was not achieved. Here, the authors report a Mycobacterium smegmatis porin A nanopore modified with a phenylboronic acid adapter for recognition of 1,2-diphenols, alditols, α-hydroxy acids and saccharides in fruits.
- Pingping Fan
- , Zhenyuan Cao
- & Shuo Huang
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Article
| Open AccessA structural and dynamic visualization of the interaction between MAP7 and microtubules
Integrated structural data show that the MAP7 microtubule binding domain stabilizes the microtubule lattice through binding along protofilaments. Both strong and weak interactions between MAP7 and the lattice extend beyond a single tubulin dimer and include the tubulin C-terminal tails.
- Agnes Adler
- , Mamata Bangera
- & Marc Baldus
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Article
| Open AccessA uniform data processing pipeline enables harmonized nanoparticle protein corona analysis across proteomics core facilities
Protein corona is crucial for the safety and efficacy of nanomedicines, and the protein composition of the corona layer is typically analysed using liquid chromatography-mass spectrometry. Here the authors report that the use of a uniform database search provides an opportunity for taking measures in good practice and quality control in protein corona research using mass spectroscopy technique.
- Hassan Gharibi
- , Ali Akbar Ashkarran
- & Morteza Mahmoudi
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Article
| Open AccessPrecise in-field molecular diagnostics of crop diseases by smartphone-based mutation-resolved pathogenic RNA analysis
On-site crop disease diagnostics is critical for precise application of pesticides. Here, the authors report an in-field molecular diagnostic tool for wheat pathogens using a nucleic acid amplification-free, gene mutation-resolved and smartphone-integrated genetic assay.
- Ting Zhang
- , Qingdong Zeng
- & Ruijie Deng
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Article
| Open AccessEnabling programmable dynamic DNA chemistry using small-molecule DNA binders
The binding of small molecules to the double stranded DNA may significantly alter its stability and functionality, which is the basis for many therapeutic and sensing applications. Here, the authors report that DNA binders can be used to program reaction pathways of a dynamic DNA reaction, where DNA strand displacement can be tuned quantitatively according to the affinity, charge, and concentrations of a given DNA binder.
- Junpeng Xu
- , Guan Alex Wang
- & Feng Li
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Article
| Open AccessDetermining the gas-phase structures of α-helical peptides from shape, microsolvation, and intramolecular distance data
It remains challenging to gauge the gas-phase structure of biomolecular ions and assess to what extent native-like structures are maintained. Here, the authors utilize Förster resonance energy transfer and ion mobility spectrometry for more stringent structural characterization of biomolecular ions.
- Ri Wu
- , Jonas B. Metternich
- & Renato Zenobi
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Article
| Open AccessAdaptable graphitic C6N6-based copper single-atom catalyst for intelligent biosensing
Catalysts with multiple and modulable reaction pathways are promising but generally hampered by inconsistent reaction conditions and negative internal interferences. Herein, the authors report an adaptable graphitic C6N6-based copper singleatom catalyst
- Qing Hong
- , Hong Yang
- & Yuanjian Zhang
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Article
| Open AccessIdentification of tagged glycans with a protein nanopore
The structural complexity of glycans seriously challenges the currently available analytical methods. Here, the authors report the identification of glycan isomers, glycans with varying chain lengths, and distinct branched glycans, via a glycan derivatization strategy and nanopore sensing.
- Minmin Li
- , Yuting Xiong
- & Guangyan Qing
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Article
| Open Access1,2,4,5-Tetrazine-tethered probes for fluorogenically imaging superoxide in live cells with ultrahigh specificity
Specific detection of cellular superoxide is challenging. Here, the authors designed 1,2,4,5-tetrazine based fluorogenic probes for specific and sensitive imaging of superoxide, and applied them in high throughput screening of modulators of oxidative stress.
- Xuefeng Jiang
- , Min Li
- & Xin Li
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Article
| Open AccessArginine-modified black phosphorus quantum dots with dual excited states for enhanced electrochemiluminescence in bioanalysis
Electrochemiluminescence is emitted via the radiative transition of a singlet or triplet excited state. Here, the authors propose an arginine modification of black phosphorus quantum dots that exhibits enhanced emission based on dual excited states.
- Siqi Yu
- , Yu Du
- & Huangxian Ju
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Article
| Open AccessComprehensive structural assignment of glycosaminoglycan oligo- and polysaccharides by protein nanopore
Glycosaminoglycans (GAGs) are highly anionic functional polysaccharides with subtle structural variations that are very difficult to differentiate. Here the authors demonstrate proof-of-concept single-molecule detection by nanopore, taking a first step towards the ultimate goal of GAG sequencing.
- Parisa Bayat
- , Charlotte Rambaud
- & Régis Daniel
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Article
| Open AccessThree-dimensional structure determination of protein complexes using matrix-landing mass spectrometry
Mass spectrometry (MS) is a powerful tool for the structural characterization of protein complexes. Here the authors offer a path for direct integration of MS and electron microscopy with a MS approach that enables grid deposition and structural preservation of gaseous protein complex ions.
- Michael S. Westphall
- , Kenneth W. Lee
- & Joshua J. Coon
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Article
| Open AccessFast microwave heating-based one-step synthesis of DNA and RNA modified gold nanoparticles
Simple methods for attaching polynucleotides to gold nanoparticles are of interest for simplifying conjugation in a range of applications. Here, the authors report a microwave heating-based method for the fast, one-step attachment of a range of thiolated or non-thiolated DNA and RNA to gold nanoparticles.
- Mengqi Huang
- , Erhu Xiong
- & Xiaoming Zhou
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Article
| Open AccessLipidomic profiling of human serum enables detection of pancreatic cancer
Patients with pancreatic cancer have a poor prognosis, more research is required to identify the disease at an earlier stage. Here, the authors use lipid profiles of blood samples and show that they can distinguish patients with pancreatic cancer from healthy controls.
- Denise Wolrab
- , Robert Jirásko
- & Michal Holčapek
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Article
| Open AccessProgrammable nano-reactors for stochastic sensing
Monitoring single molecule chemical reactions can be difficult and nanopore based strategies which have shown promise are technically challenging. Here, the authors report on a technique which allows for the direct observation of different reactions and demonstrate the ability to distinguish clinically relevant analogues.
- Wendong Jia
- , Chengzhen Hu
- & Shuo Huang
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Article
| Open AccessA kinetically controlled platform for ligand-oligonucleotide transduction
Ligand-oligonucleotide interactions can integrate both small molecules and proteins into nucleic acid-based circuits. Here the authors design ligand-aptamer complexes to control strand-displacement reactions for versatile ligand transduction.
- Qiu-Long Zhang
- , Liang-Liang Wang
- & Liang Xu
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Article
| Open AccessA plug-and-play platform of ratiometric bioluminescent sensors for homogeneous immunoassays
Many current immunoassays require multiple washing, incubation and optimization steps. Here the authors present Ratiometric Plug-and-Play Immunodiagnostics (RAPPID), a generic assay platform that uses ratiometric bioluminescent detection to allow sandwich immunoassays to be performed directly in solution.
- Yan Ni
- , Bas J. H. M. Rosier
- & Maarten Merkx
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Article
| Open AccessGeometrically encoded SERS nanobarcodes for the logical detection of nasopharyngeal carcinoma-related progression biomarkers
SERS assays have potential for multiplexed detection of biomarkers but differentiation of SERS tags remains a challenge. Here, the authors report the creation of 14 distinct geometrically controlled metal carbonyl tags and demonstrate multiplexed detection of nasopharyngeal carcinoma biomarkers from patient blood.
- Duo Lin
- , Chang-Lin Hsieh
- & Kien Voon Kong
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Article
| Open AccessSingle-cell lipidomics with high structural specificity by mass spectrometry
Analyzing the lipidomes of single cells remains a challenge. Here, the authors present a strategy to identify class, fatty acyl-chain, C=C locations and sn-positions of lipids in single cells, and use their method to identify individual gefitinib-resistant cells in a wild-type lung cancer cell population.
- Zishuai Li
- , Simin Cheng
- & Zheng Ouyang
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Article
| Open AccessCellular macromolecules-tethered DNA walking indexing to explore nanoenvironments of chromatin modifications
Investigation of spatial organization and relationships of biomolecules in cellular nanoenvironments is necessary to understand essential biological processes, but methodologically challenging. Here, the authors report cellular macromolecules-tethered DNA walking indexing (Cell-TALKING) to probe the nanoenvironments of DNA modifications around histone post-translational modifications, and explore the nanoenvironments in different cancer cell lines and clinical specimens.
- Feng Chen
- , Min Bai
- & Yongxi Zhao
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Article
| Open AccessOptical tweezers-controlled hotspot for sensitive and reproducible surface-enhanced Raman spectroscopy characterization of native protein structures
It is currently challenging to identify protein structures at low concentrations. Here the authors report optical tweezers-coupled Raman spectroscopy to generate tunable and reproducible SERS enhancements with single-molecule level sensitivity and use the method to detect protein structural features.
- Xin Dai
- , Wenhao Fu
- & Jinqing Huang
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Article
| Open AccessAnalysis of inositol phosphate metabolism by capillary electrophoresis electrospray ionization mass spectrometry
Myo-Inositol phosphates (InsPs) and pyrophosphates (PP-InsPs) are important second messengers but their analysis remains challenging. Here, the authors develop a capillary electrophoresis-mass spectrometry method for the identification and quantitation of InsP and PP-InsP isomers in cells and tissues.
- Danye Qiu
- , Miranda S. Wilson
- & Henning J. Jessen
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Article
| Open AccessClient proximity enhancement inside cellular membrane-less compartments governed by client-compartment interactions
Membrane-less organelles or compartments are considered to be dynamic reaction centers for spatiotemporal control of diverse cellular processes. Here authors report quantitative measurements of changes in protein interactions for the proteins recruited into membrane-less compartments (termed client proteins) in living cells.
- Daesun Song
- , Yongsang Jo
- & Yongwon Jung
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Article
| Open AccessSize-selective molecular recognition based on a confined DNA molecular sieve using cavity-tunable framework nucleic acids
Size-selective discrimination is an issue in biosensing. Here, the authors report on a size selective DNA nanocage which excludes agents based on size and protects the probes against degradation, and demonstrate the discrimination between mature and precursor miRNA.
- Xiaoyi Fu
- , Guoliang Ke
- & Weihong Tan
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Article
| Open AccessProgramming bulk enzyme heterojunctions for biosensor development with tetrahedral DNA framework
Tetrahedral DNA framework-enabled bulk enzyme heterojunctions have been used to program biosensor interfaces. Here, the authors use DNA tetrahedrons to tether enzymes of an enzymatic cascade to gold electrodes, hence raising them over the bulk solution, which led to improved kinetics and sensitivity.
- Ping Song
- , Juwen Shen
- & Chunhai Fan
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Article
| Open AccessStudying biomolecular folding and binding using temperature-jump mass spectrometry
Native mass spectrometry allows monitoring the folding and interactions of multiple coexisting species but its temporal resolution is traditionally limited. Here, the authors develop a temperature-jump electrospray source for mass spectrometry that enables fast kinetics experiments at different temperatures.
- Adrien Marchand
- , Martin F. Czar
- & Renato Zenobi
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Article
| Open AccessH2S-activatable near-infrared afterglow luminescent probes for sensitive molecular imaging in vivo
Afterglow imaging probes are of interest for in vivo imaging due to high signal-to-background ratios. Here, the authors report on an afterglow nanoparticle which is activated by hydrogen sulphide and demonstrate the measurement of hydrogen sulphide levels and the labelling of hepatic cancer specimens in vivo.
- Luyan Wu
- , Yusuke Ishigaki
- & Deju Ye
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Article
| Open AccessLarge-scale lipid analysis with C=C location and sn-position isomer resolving power
Coupling photochemical derivatization with tandem mass spectrometry enables C=C-isomer resolved lipidomics. Here, the authors further develop this approach into a shotgun lipidomics workflow that allows simultaneous characterization of lipid C=C locations and sn-positions in complex biological samples.
- Wenbo Cao
- , Simin Cheng
- & Xiaoxiao Ma
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Article
| Open AccessTrapped ion mobility spectrometry and PASEF enable in-depth lipidomics from minimal sample amounts
Trapped ion mobility (TIMS)-mass spectrometry with parallel accumulation-serial fragmentation (PASEF) facilitates high-sensitivity proteomics experiments. Here, the authors expand TIMS and PASEF to small molecules and demonstrate fast and comprehensive lipidomics of low biological sample amounts.
- Catherine G. Vasilopoulou
- , Karolina Sulek
- & Florian Meier
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Article
| Open AccessSimultaneous multi-signal quantification for highly precise serodiagnosis utilizing a rationally constructed platform
Single channel detection methods often suffer from false positives when analysing biological samples. Here, the authors report on the development of a three-channel detection device for measuring hydrogen sulphide in serum and demonstrate application in an in vivo model.
- Yuxin Liu
- , Zheng Wei
- & Zhanfang Ma
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Comment
| Open AccessThe ever expanding scope of electrospray mass spectrometry—a 30 year journey
John Fenn’s electrospray mass spectrometry (ESMS) was awarded the chemistry Nobel Prize in 2002 and is now the basis of the entire field of MS-based proteomics. Technological progress continues unabated, enabling single cell sensitivity and clinical applications.
- Matthias Mann
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Article
| Open AccessSmall molecule electro-optical binding assay using nanopores
Nanopore detection of small molecules can be improved using molecular carriers, but separating a small analyte from the carrier signal can be challenging. Here the authors address this challenge using simultaneous electrical and optical readout in nanopore sensing to detect small molecules and quantify binding affinities.
- Shenglin Cai
- , Jasmine Y. Y. Sze
- & Joshua B. Edel
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Article
| Open AccessScalable dissolution-dynamic nuclear polarization with rapid transfer of a polarized solid
Dissolution-dynamic nuclear polarization is able to enhance nuclear magnetic resonance signals, but requires complex procedures to generate hyperpolarized nuclear spins. Here the authors establish a fast and facile method to transfer hyperpolarized samples into the liquid solution where the measurement is performed.
- Karel Kouřil
- , Hana Kouřilová
- & Benno Meier
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Article
| Open AccessControl of capillary behavior through target-responsive hydrogel permeability alteration for sensitive visual quantitative detection
DNA hydrogels have received considerable attention in analytical science but limitations still exist in the applications of intelligent hydrogels. Here, the authors describe a DNA hydrogel sensor for quantitative detection of cocaine based on the permeability change in a DNA hydrogel film.
- Yansheng Li
- , Yanli Ma
- & Yongqiang Wen
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Article
| Open AccessAnti-quenching NIR-II molecular fluorophores for in vivo high-contrast imaging and pH sensing
Fluorophores operating in the second near-infrared window suffer from solvatochromism-caused fluorescence quenching in biological aqueous solution. Here, the authors synthesized a series of pH-responsive pentamethine cyanine fluorophores that afford stable absorption/emission beyond 1000 nm.
- Shangfeng Wang
- , Yong Fan
- & Fan Zhang
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Article
| Open AccessRapid one-step 18F-radiolabeling of biomolecules in aqueous media by organophosphine fluoride acceptors
The synthesis of 18F-labeled positron emission tomography (PET) tracers is difficult and typically requires anhydrous conditions. Here, the authors developed organophosphine precursors that allow for quick, high-yield synthesis of 18F-labeled probes in either organic solvents or aqueous media.
- Huawei Hong
- , Lei Zhang
- & Zijing Li
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Article
| Open AccessIon mobility conformational lipid atlas for high confidence lipidomics
The biological functions of lipids critically depend on their highly diverse molecular structures. Here, the authors determine the mass-resolved collision cross sections of 456 sphingolipid and glycerophospholipid species, providing a reference for future structural lipidomics studies.
- Katrina L. Leaptrot
- , Jody C. May
- & John A. McLean
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Article
| Open AccessElectrochromic semiconductors as colorimetric SERS substrates with high reproducibility and renewability
Electrochromic technology has diverse cutting-edge applications, but it has never been used to overcome the critical problems in the field of surface-enhanced Raman scattering (SERS). Here, the authors demonstrate a generic electrochromic strategy for ensuring the reproducibility and renewability of SERS substrates.
- Shan Cong
- , Zhen Wang
- & Zhigang Zhao
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Article
| Open AccessUltrasensitive detection of miRNA with an antimonene-based surface plasmon resonance sensor
Label-free molecular-level quantification of MicroRNA (miRNA) remains challenging. Here, the authors develop a new surface plasmon resonance sensor based on two-dimensional nanomaterial of antimonene for the specific label-free detection of clinically relevant biomarkers such as miRNA-21 and miRNA-155.
- Tianyu Xue
- , Weiyuan Liang
- & Qiaoliang Bao
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Article
| Open AccessMonitoring drug nanocarriers in human blood by near-infrared fluorescence correlation spectroscopy
While nanocarrier-based drug delivery is a promising therapeutic approach, in situ characterization of drug nanocarriers in blood remains difficult. Here, the authors demonstrate how the fluorescence correlation spectroscopy can be used to directly characterize drug nanocarriers in flowing blood.
- Inka Negwer
- , Andreas Best
- & Kaloian Koynov
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Article
| Open AccessDistinct functional elements for outer-surface anti-interference and inner-wall ion gating of nanochannels
Nanochannels are often modified with functional elements, but most studies have focused on functionalizing only the inner wall. Here, the authors design nanochannels with distinct chemical modifications on the inner and outer surfaces, providing a route to dual-function channels.
- Pengcheng Gao
- , Qun Ma
- & Fan Xia
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Article
| Open AccessManipulating and visualizing the dynamic aggregation-induced emission within a confined quartz nanopore
The difficulty in recovering the aggregation-induced emission fluorogens (AIEgens) to the initial dispersed state upon illuminating has limited their applications. Here, the authors employ the confined space in the quartz nanopore to achieve a nanopore-size dependent restriction of AIEgens.
- Yi-Lun Ying
- , Yuan-Jie Li
- & He Tian
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Article
| Open AccessLiquid-state quantitative SERS analyzer on self-ordered metal liquid-like plasmonic arrays
The design and application of a liquid interfacial plasmonic platform promises for practical applications of surface-enhanced Raman scattering (SERS). Here, the authors report a reversible chloroform/water encasing strategy to self-assemble metal liquid-like 3D gold nanorod arrays with attractive SERS capability.
- Li Tian
- , Mengke Su
- & Weihong Tan
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Article
| Open AccessSurveying silicon nitride nanopores for glycomics and heparin quality assurance
The complexity of polysaccharides significantly complicates their analysis in comparison to other biopolymers. Here, the authors demonstrate that solid-state silicon nitride nanopore sensors can be used to reliably detect native polysaccharides and to perform a simple quality assurance assay on a polysaccharide therapeutic, heparin.
- Buddini Iroshika Karawdeniya
- , Y. M. Nuwan D. Y. Bandara
- & Jason R. Dwyer
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Article
| Open AccessSimultaneous and stoichiometric purification of hundreds of oligonucleotides
Chemically synthesized DNA oligonucleotides (oligos) require purification to remove truncated species. Here, the authors developed a high-throughput method for oligo purification that also normalises the concentrations of the oligos in the final samples.
- Alessandro Pinto
- , Sherry X. Chen
- & David Yu Zhang
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Article
| Open AccessLight-induced formation of partially reduced oxygen species limits the lifetime of photosystem 1-based biocathodes
Photobiodevices use photosynthetic proteins such as those of the photosystem 1 (PS1) to enable light-induced charge separation, but they suffer from limited long-term stability. Here authors employ scanning photoelectrochemical microscopy on a PS1 biocathode and find that several pathways generate oxygen radicals.
- Fangyuan Zhao
- , Steffen Hardt
- & Felipe Conzuelo