Featured
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| Open AccessRapid room-temperature phosphorescence chiral recognition of natural amino acids
Chiral recognition of amino acids with luminescence, despite its advantages, is usually slow and lacks generality. Here, the authors demonstrate that L-phenylalanine derived benzamide can manifest the structural difference between the natural, left-handed amino acid and its right-handed counterpart via the difference in room-temperature phosphorescence, irrespective of the specific chemical structure.
- Xiaoyu Chen
- , Renlong Zhu
- & Guoqing Zhang
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Article
| Open AccessAlkyne-tagged SERS nanoprobe for understanding Cu+ and Cu2+ conversion in cuproptosis processes
Simultaneously quantifying mitochondrial Cu+ and Cu2+ levels is vital for understanding the molecular mechanism of mitochondria-related biological events. Here the authors report an alkynyl-labeled SERS probe to simultaneously monitor free Cu+ and Cu2+ in mitochondria, and unveil their roles during ischemia and cuproptosis processes.
- Sihan Zhang
- , Yuxiao Mei
- & Yang Tian
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Article
| Open AccessAggregation induced emission dynamic chiral europium(III) complexes with excellent circularly polarized luminescence and smart sensors
Chiral luminescent materials are of increasing interest in various applications, but achieving a desirable balance of properties can be challenging. Here, the authors report the development of Eu-based complexes with chiral luminescence and aggregation induced emission.
- Yun-Lan Li
- , Hai-Ling Wang
- & Hua-Hong Zou
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Article
| Open AccessAutonomous closed-loop mechanistic investigation of molecular electrochemistry via automation
Electrochemical research often requires stringent combinations of experimental parameters that are demanding to manually locate. Here the authors report an autonomous electrochemical platform that implements an adaptive, closed-loop workflow for mechanistic investigation of molecular electrochemistry.
- Hongyuan Sheng
- , Jingwen Sun
- & Chong Liu
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Article
| Open AccessForward-predictive SERS-based chemical taxonomy for untargeted structural elucidation of epimeric cerebrosides
SERS-based chemical taxonomy is attractive for practical SERS applications where the identity and concentration of analytes are unknown. Here, the authors demonstrate a machine learning framework for classifying “unknown” molecules that lie outside the boundaries of the models used.
- Emily Xi Tan
- , Shi Xuan Leong
- & Xing Yi Ling
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Article
| Open AccessPhotoswitchable polyynes for multiplexed stimulated Raman scattering microscopy with reversible light control
Bioimaging with photocontrol and multiplexing capability is vital for studying cellular interactions and dynamics, but multiplexed stimulated Raman scattering (SRS) imaging with reversible photocontrol is elusive. Here, the authors report SRS microscopy with Carbow-switch enabling multiplexed SRS imaging and tracking in live cells with reversible photocontrol and high spatiotemporal selectivity.
- Yueli Yang
- , Xueyang Bai
- & Fanghao Hu
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Article
| Open AccessUltra-photostable small-molecule dyes facilitate near-infrared biophotonics
Near-infrared small molecule dyes are attractive in biophotonics, but generally rely on expanded aromatic structures to achieve this redshift. Here the authors report the use of a ground state antiaromatic strategy for 14 aminofluorene dyes, and their use in imaging kidney injury.
- Kui Yan
- , Zhubin Hu
- & Fan Zhang
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Article
| 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 AccessRectifying artificial nanochannels with multiple interconvertible permeability states
Transmembrane channels have inspired the development of biomimetic channels. Here, the authors present a class of artificial nanochannels based on DNAzyme-functionalized glass nanopipettes to allow for the control of channel permeability.
- Ruocan Qian
- , Mansha Wu
- & Yi Lu
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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 AccessIntegrating single-cell and spatially resolved transcriptomic strategies to survey the astrocyte response to stroke in male mice
Astrocytes adopt diverse states in response to brain injuries. Here, the authors develop a platform for spatially resolved, single-cell transcriptomics and proteomics, called tDISCO (tissue-digital microfluidic isolation of single cells for -Omics) to uncover the spatial boundaries of molecularly distinct reactive astrocyte populations in stroke.
- Erica Y. Scott
- , Nickie Safarian
- & Maryam Faiz
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Article
| Open AccessEfficient catalyst-free N2 fixation by water radical cations under ambient conditions
The growth and sustainable development of humanity is heavily dependent upon N2 fixation. Herein, authors developed an ambient catalyst-free disproportionation of N2 by water plasma to yield economically valuable nitroxyl and hydroxylamine products.
- Xiaoping Zhang
- , Rui Su
- & Huanwen Chen
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Article
| Open AccessPick-up single-cell proteomic analysis for quantifying up to 3000 proteins in a Mammalian cell
Single-cell proteomics is of fundamental importance to capture biological heterogeneity, while limited in proteome depth. Here, the authors develop a pick-up single-cell proteomic analysis (PiSPA) workflow to achieve a deep coverage of quantifying up to 3000 protein groups in a mammalian cell.
- Yu Wang
- , Zhi-Ying Guan
- & Qun Fang
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Article
| Open AccessAn integrated self-optimizing programmable chemical synthesis and reaction engine
A limitation of robotic platforms in chemistry is the lack of feedback loops to adjust the conditions in-operando. Here the authors present a dynamically programmable robotic system that uses sensors for real-time adaptation, achieving yield improvements in syntheses and discovering new molecules.
- Artem I. Leonov
- , Alexander J. S. Hammer
- & Leroy Cronin
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Article
| Open AccessVisualization-enhanced under-oil open microfluidic system for in situ characterization of multi-phase chemical reactions
Under-oil open microfluidic systems have potential for studying multi-phase chemical reactions but have so far demonstrated largely only for biological applications. Here, the authors report the development of a system for in situ characterization of gas-liquid reactions by Raman spectroscopy.
- Qiyuan Chen
- , Hang Zhai
- & Bu Wang
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Article
| Open AccessMicropillar arrays, wide window acquisition and AI-based data analysis improve comprehensiveness in multiple proteomic applications
Obtaining a comprehensive proteomic profile for complex samples is still an elusive task. Here, the authors present an LC-MS/MS workflow including micropillar arrays, wide isolation windows and AI-based data analysis to boost proteomic coverage and throughput for multiple proteomic samples.
- Manuel Matzinger
- , Anna Schmücker
- & Rupert L. Mayer
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Article
| Open AccessEarly onset diagnosis in Alzheimer’s disease patients via amyloid-β oligomers-sensing probe in cerebrospinal fluid
In this work, the authors characterize a small molecule fluorescent probe pioneering early diagnosis of Alzheimer’s disease through identification of amyloid-β oligomers in patients’ cerebrospinal fluid, demonstrating potential for clinical application.
- Jusung An
- , Kyeonghwan Kim
- & Jong Seung Kim
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Article
| Open AccessNoise learning of instruments for high-contrast, high-resolution and fast hyperspectral microscopy and nanoscopy
Improving signal to noise ratio of Raman spectra is vital for the application. Here, authors show a noise learning method that learns the noise feature of a spectrometer. This improves the signal to noise ratio and makes deep learning to be instrument dependent instead of sample dependent.
- Hao He
- , Maofeng Cao
- & Bin Ren
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Article
| Open AccessRapid and visual identification of β-lactamase subtypes for precision antibiotic therapy
The rapid identification of drug-resistant bacteria is vital for effective treatment and to avoid antibiotic misuse. Here authors report a paper-based sensor which utilises chromogenic carbapenem and cephalosporin substrates for the identification and discrimination of β-lactamase subtypes.
- Wenshuai Li
- , Jingqi Li
- & Dingbin Liu
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Article
| Open AccessRatiometric fluorescent sensing of pyrophosphate with sp³-functionalized single-walled carbon nanotubes
Inorganic pyrophosphate is a key molecule in many biological processes. Here, the authors develop an optical sensor that enables its ratiometric detection in the near infrared with functionalized single-walled carbon nanotubes.
- Simon Settele
- , C. Alexander Schrage
- & Jana Zaumseil
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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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Comment
| Open AccessImproving reproducibility of photocatalytic reactions—how to facilitate broad application of new methods
Photocatalysis, as a powerful tool for synthetic transformations, has the potential to impact industrial applications. In this commentary, we discuss the challenges and requirements with respect to reproducing published photocatalytic reactions in the (life science) industry.
- Santiago Cañellas
- , Manuel Nuño
- & Elisabeth Speckmeier
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Article
| Open AccessDirect identification of interfacial degradation in blue OLEDs using nanoscale chemical depth profiling
Understanding the degradation mechanism of organic light-emitting diodes is essential to improve device performance and stability. Here, authors present a high-resolution diagnostic method to obtain molecular information with 7-nm depth resolution and analyse devices at different degradation levels.
- Gustavo F. Trindade
- , Soohwan Sul
- & Ian S. Gilmore
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Article
| Open AccessDirect probing of single-molecule chemiluminescent reaction dynamics under catalytic conditions in solution
Research into the dynamics of chemical reactions at the single-molecule level is a pivotal undertaking. Here, the authors present a direct investigation of the chemiluminescent reaction dynamics of single molecules in solution, providing spatiotemporally resolved insights into chemical reactions.
- Ziqing Zhang
- , Jinrun Dong
- & Jiandong Feng
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Article
| Open AccessOn-tissue dataset-dependent MALDI-TIMS-MS2 bioimaging
There is a need for dataset-dependent MS2 acquisition in trapped ion mobility spectrometry imaging. Here the authors report spatial ion mobility-scheduled exhaustive fragmentation (SIMSEF) which enables on-tissue metabolite and lipid annotation in mass spectrometry bioimaging studies, and use this to visualise the chemical space in rat brains.
- Steffen Heuckeroth
- , Arne Behrens
- & Robin Schmid
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Article
| Open AccessStructural characterization of tin in toothpaste by dynamic nuclear polarization enhanced 119Sn solid-state NMR spectroscopy
Stannous fluoride (SnF2) is a common fluoride source and antimicrobial agent used in commercial toothpaste products. Here, the authors show how dynamic nuclear polarization can be used to perform 119Sn nuclear magnetic resonance spectroscopy experiments that probe the molecular structure of tin ions in commercial toothpastes.
- Rick W. Dorn
- , Scott L. Carnahan
- & Aaron J. Rossini
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Article
| Open AccessLocalized cardiac small molecule trajectories and persistent chemical sequelae in experimental Chagas disease
The impact of antiparasitic treatment on local tissue responses in the case of chronic Chagas disease (caused by Trypanosoma cruzi infection) is not well understood. Authors provide insight into clinical treatment failure and drivers of post-infectious conditions.
- Zongyuan Liu
- , Rebecca Ulrich vonBargen
- & Laura-Isobel McCall
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Article
| Open AccessSialic acid O-acetylation patterns and glycosidic linkage type determination by ion mobility-mass spectrometry
O-acetylation is a common modification of sialic acids. Here, a library of synthetic O-acetylated sialosides made it possible to develop an ion mobility mass spectrometry (IM-MS) approach that can elucidate exact O-acetylation patterns and glycosidic linkage types of sialosides isolated from biological samples.
- Gaёl M. Vos
- , Kevin C. Hooijschuur
- & Geert-Jan Boons
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Article
| Open AccessMolecular imprinting-based indirect fluorescence detection strategy implemented on paper chip for non-fluorescent microcystin
Fluorescence analysis is a fast and sensitive method for the trace detection of environmental toxins, but it remains challenging to develop a fluorescence method for detecting nonfluorescent toxins. Here, the authors report an indirect fluorescent sensing strategy for the rapid, selective and sensitive detection of the non-fluorescent microcystin as a model target.
- Bowei Li
- , Ji Qi
- & Lingxin Chen
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Article
| Open AccessCapturing nascent extracellular vesicles by metabolic glycan labeling-assisted microfluidics
Temporally sorting EV populations is hard. Here the authors report a microfluidic-based strategy to enable selective isolation of nascent EVs by using azido groups to act as a timestamp for click chemistry labelling: they apply this to mouse models of anti-PD-L1 immunotherapy.
- Qiuyue Wu
- , Wencheng Wang
- & Yanling Song
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Article
| Open AccessCell-inspired design of cascade catalysis system by 3D spatially separated active sites
Cells contain isolated compartments that spatially confine different enzymes, enabling high-efficiency enzymatic cascade reactions. Herein, the authors report a cell-inspired design of biomimetic cascade catalysis system by immobilizing Fe single atoms and Au nanoparticles on the inner and outer layers of three-dimensional nanocapsules, respectively, to enable highly selective colorimetric glucose detection.
- Qiuping Wang
- , Kui Chen
- & Yuen Wu
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Article
| Open AccessInfrared spectroscopic laser scanning confocal microscopy for whole-slide chemical imaging
Chemical imaging, including infrared spectroscopic microscopy with molecular sensitivity, is useful for label-free biomedical analyses, but is limited by slow speed and poor image quality. Here, the authors design a fast mid-infrared microscope with low noise and high spatial resolution for high-throughput imaging of whole slides.
- Kevin Yeh
- , Ishaan Sharma
- & Rohit Bhargava
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Article
| Open AccessIdentifying and preventing degradation in flavin mononucleotide-based redox flow batteries via NMR and EPR spectroscopy
Aqueous organic redox-flow batteries are known to suffer capacity loss via degradation of the redox-active species. Here, the authors use in situ methods to study the electrolyte flavin mononucleotide, identifying a redox mediator mechanism that mitigates capacity loss and a route to prevent its degradation.
- Dominic Hey
- , Rajesh B. Jethwa
- & Clare P. Grey
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Article
| Open AccessAtomic-level structure determination of amorphous molecular solids by NMR
The atomic-level ensemble structure of an amorphous form of a drug is determined by combining NMR experiments with molecular dynamics simulations and machine-learned chemical shifts. The structure explains the stabilization of the amorphous form.
- Manuel Cordova
- , Pinelopi Moutzouri
- & Lyndon Emsley
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Article
| Open AccessSHARPER-DOSY: Sensitivity enhanced diffusion-ordered NMR spectroscopy
Since its discovery, the sensitivity of Nuclear Magnetic Resonance has increased steadily. Here the authors report on a liquid-state NMR methodology that increases the sensitivity of the diffusion coefficient measurements 10–100- fold, allowing to use microgram quantities of compounds, while reducing the measurement time to few minutes.
- George Peat
- , Patrick J. Boaler
- & Dušan Uhrín
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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 AccessDeep-profiling of phospholipidome via rapid orthogonal separations and isomer-resolved mass spectrometry
The existence of large number of isomers poses challenges for lipidomic analysis. The authors integrate hydrophilic interaction liquid chromatography, trapped ion mobility, and isomer-resolved MS/MS into a single system, enabling deep profiling of phospholipidomes at fast speed and wide coverage.
- Tian Xia
- , Feng Zhou
- & Yu Xia
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Article
| Open AccessDynamic imaging of interfacial electrochemistry on single Ag nanowires by azimuth-modulated plasmonic scattering interferometry
Direct visualization of the chemical dynamics of surfaces in solution is essential to gain mechanistic insights into nanocatalysis and electrochemistry. Here, the authors demonstrate the imaging of dynamic interfacial changes on a single nanowire during chemical reactions using azimuthally modulated plasmonic scattering interferometry.
- Gang Wu
- , Chen Qian
- & Xian-Wei Liu
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Article
| Open AccessHighly efficient platelet generation in lung vasculature reproduced by microfluidics
Highly efficient generation of platelets in the vasculature. Here, Zhao et al. show that the mouse platelet precursor cell, megakaryocytes, generate physiological numbers of functional platelets when passaged repeatedly through pulmonary vasculature.
- Xiaojuan Zhao
- , Dominic Alibhai
- & Alastair W. Poole
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Article
| Open AccessMultinuclear 1D and 2D NMR with 19F-Photo-CIDNP hyperpolarization in a microfluidic chip with untuned microcoil
The main limitations in NMR techniques are low sensitivity and the requirement for complex instrumentation. Here the authors show that a microfluidic chip with a single untuned planar spiral microcoil, combined with laser-light induced hyperpolarization, allows for multidimensional and heteronuclear Nuclear Magnetic Resonance spectroscopy on picomole quantities of material.
- M. Victoria Gomez
- , Sander Baas
- & Aldrik H. Velders
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Article
| Open AccessUltra-fast and accurate electron ionization mass spectrum matching for compound identification with million-scale in-silico library
Accuracy loss and slow speed affect the identification of compounds through matching of mass spectra using a large-scale spectral library. Here the authors use Word2vec spectral embedding and hierarchical navigable small-world graph to improve accuracy and speed of spectral matching on their own million-scale in-silico library.
- Qiong Yang
- , Hongchao Ji
- & Zhimin Zhang
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Article
| Open AccessData fusion and multivariate analysis for food authenticity analysis
Using two different mass spectrometric platforms, authors demonstrate how metabolomic data fusion and multivariate analysis can be used to accurately identify the geographic origin and production method of salmon.
- Yunhe Hong
- , Nicholas Birse
- & Christopher T. Elliott
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Article
| Open AccessRetention time prediction for chromatographic enantioseparation by quantile geometry-enhanced graph neural network
Chromatographic enantioseparation requires tedious trials to find proper experimental conditions. Here, the authors construct a deep learning model to predict retention times of chiral molecules and obtain the separation probability under given conditions.
- Hao Xu
- , Jinglong Lin
- & Fanyang Mo
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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