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| Open AccessMolecular probes for tracking lipid droplet membrane dynamics
Lipid droplets (LDs) and their membrane proteins play essential roles in many biological processes, but the monolayer lipid membrane of LDs has not been extensively studied due to the lack of suitable molecular probes. Here, the authors report an LD membrane labelling pro-probe called LDM, which, upon activation by the HClO/ClO− microenvironment that surrounds LDs, undergoes a color change and releases LDM-OH probe that binds to LD membrane proteins.
- Lingxiu Kong
- , Qingjie Bai
- & Qixin Chen
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Article
| Open AccessRecovering nutrients and unblocking the cake layer of an electrochemical anaerobic membrane bioreactor
Recovering resources from wastewater sources is an important sustainable development strategy. Here, authors build an electrochemical resource-recovery anaerobic membrane bioreactor for the simultaneous full recovery of carbon, nitrogen, and phosphorus, while demonstrating membrane fouling mitigation.
- Yuhan Zhang
- , Yongbin Wang
- & Jiuhui Qu
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Article
| Open AccessPutting the squeeze on valence tautomerism in cobalt-dioxolene complexes
While thermally- and photo-induced valence tautomerism, which is stimulated intramolecular electron transfer between a metal and coordinated redox-active ligand, has been explored extensively, less is known about pressure-induced valence tautomerism. Here, the authors report pressure-triggered valence tautomerism in a thermally inactive cobalt complex.
- Aston Summers
- , F. Zahra M. Zahir
- & Stephen A. Moggach
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Article
| Open AccessAtomically dispersed recognition unit for selective in vivo photoelectrochemical medicine detection
Continuous and long-term monitoring of medicines in biological systems could offer personalized pharmacokinetic reports but is challenging due to the complexity of the biological environment in living organisms. Here, the authors present a photoelectrochemical biosensor with single atom Cu on TiO2-x as recognition unit for selective, precise, long-term tetracycline monitoring in living organisms.
- Xiankui Xu
- , Dawei Xu
- & Zhonghai Zhang
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Article
| Open AccessCell fixation improves performance of in situ crosslinking mass spectrometry while preserving cellular ultrastructure
Crosslinking mass spectrometry protocols applied directly to cells can distort the spatial proteome. Here, the authors show that prefixing the cell with high concentrations of formaldehyde can prevent this, while simultaneously increasing crosslink yield and supporting the use of any type of crosslinker.
- Andrew R. M. Michael
- , Bruno C. Amaral
- & David C. Schriemer
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Article
| Open AccessDesigning chemical systems for precision deuteration of medicinal building blocks
Deuteration of active pharmaceutical ingredients is increasingly applied as the isosteric and isotopic replacement can modulate the pharmacokinetic profile, without necessarily having to alter the overall synthetic strategy toward the compound of interest. Here, the authors show manifold deuterations of piperidines and apply molecular rotational resonance (MRR) spectroscopy as a methodology to distinguish isotopomers within a distribution of products.
- Jonathan D. Dabbs
- , Caleb C. Taylor
- & W. Dean Harman
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Article
| Open AccessArtificial olfactory memory system based on conductive metal-organic frameworks
A chemical infrastructure for integrating sensing and memory and exhibiting short- and long-term memory responses to alcohols and aldehydes through an artificial olfactory memory system is realized with conductive metal-organic framework Ce-HHTP.
- Xiaomeng Yin
- , Hao Zhang
- & Tie Wang
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Article
| Open AccessDeep learning prediction of electrospray ionization tandem mass spectra of chemically derived molecules
Chemical derivatization is widely used, but the lack of reference spectra of chemically derived molecules (CDMs) hinders their identification. Here, the authors describe a deep learning approach enabling accurate prediction of ESIMS/MS spectra for CDMs.
- Bin Chen
- , Hailiang Li
- & Feng Li
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Article
| Open AccessInflammation-free electrochemical in vivo sensing of dopamine with atomic-level engineered antioxidative single-atom catalyst
Electrochemical methods are promising for monitoring neurochemical dynamics, but are limited by inflammation effects from electrode implantation. Here, the authors report the development of a single-atom catalyst that acts both as an antioxidative nanozyme and an electrode material for the inflammation-free sensing of dopamine in the brain.
- Xiaolong Gao
- , Huan Wei
- & Lanqun Mao
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Article
| Open AccessSingle-molecule digital sizing of proteins in solution
Physical characterisation of proteins is challenging. Here the authors report single-molecule microfluidic diffusional sizing (smMDS) to enable calibration-free single-molecule diffusional-sizing based monitoring of protein hydrodynamic radii even within heterogenous multicomponent mixtures.
- Georg Krainer
- , Raphael P. B. Jacquat
- & Tuomas P. J. Knowles
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Article
| Open AccessTrace element detection in anhydrous minerals by micro-scale quantitative nuclear magnetic resonance spectroscopy
Nominally anhydrous minerals composing Earth’s and planetary rocks incorporate microscopic amounts of volatiles whose distribution affects their physical properties. Here the authors present an approach for trace-element quantification using micro-scale Nuclear Magnetic Resonance spectroscopy.
- Yunhua Fu
- , Renbiao Tao
- & Thomas Meier
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Article
| Open AccessFast and deep phosphoproteome analysis with the Orbitrap Astral mass spectrometer
Protein phosphorylation plays critical roles in myriad cell processes. In this work, the authors apply new mass spectrometer technology to detect and quantify tens of thousands of protein phosphorylation sites within one hour or less of analysis. This technology has potential to greatly accelerate biological discovery.
- Noah M. Lancaster
- , Pavel Sinitcyn
- & Joshua J. Coon
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Article
| Open AccessElucidation of hemilabile-coordination-induced tunable regioselectivity in single-site Rh-catalyzed heterogeneous hydroformylation
Unveiling the regulatory mechanism of regioselectivity in hydroformylation has been a significant challenge. Here the authors successfully demonstrate how hemilabile coordination influences regioselectivity by employing various in situ techniques.
- Benhan Fan
- , Miao Jiang
- & Yunjie Ding
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Article
| Open AccessCovalent penicillin-protein conjugates elicit anti-drug antibodies that are clonally and functionally restricted
Penicillin and other β-lactam drugs form protein adducts that can facilitate allergic and other drug-directed responses. Here, Deimel et al. describe the pharmacokinetic, immunologic and structural determinants of anti-penicillin antibodies.
- Lachlan P. Deimel
- , Lucile Moynié
- & Quentin J. Sattentau
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Article
| Open AccessReconfiguration of organic electrochemical transistors for high-accuracy potentiometric sensing
The translation of transistor-based sensor technologies is limited by unreliable potentiometric sensing. Here, the authors propose a transistor configuration that eliminates the measurement inaccuracies associated with electrochemical transistor-based potentiometric sensors.
- Luca Salvigni
- , Prem Depan Nayak
- & Sahika Inal
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Article
| Open AccessDesigned 2D protein crystals as dynamic molecular gatekeepers for a solid-state device
Vijayakumar and coworkers report the integration of a designed, 2D crystalline protein assembly as a dynamic gatekeeper into mesoporous silicon photonic crystals for the selective sensing of hydrogen cyanide
- Sanahan Vijayakumar
- , Robert G. Alberstein
- & F. Akif Tezcan
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Article
| Open AccessDielectrophoretic bead-droplet reactor for solid-phase synthesis
The immobilization of one reactant on a solid support makes interfacing of reagents a critical challenge in solid-phase synthesis. Here, authors combine dielectrophoresis and droplet microfluidics to encapsulate and eject individual beads out of reagent droplets for improved reaction fidelity.
- Punnag Padhy
- , Mohammad Asif Zaman
- & Lambertus Hesselink
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Article
| Open AccessA single-particle mechanofluorescent sensor
A mechano-fluorescence sensor system using polydiacetylene (PDA) particles monitors mechanical stresses in microchannels mimicking stenotic vessels, with fluorescence varying by fluid viscosity and particle collisions, aiding in in-vitro simulations.
- Narges Ahmadi
- , Jieun Lee
- & Bum Jun Park
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Article
| Open AccessWide-energy programmable microwave plasma-ionization for high-coverage mass spectrometry analysis
Ion source technology in mass spectrometry still has limitations in analyte coverage. Here, the authors present a wide-energy programmable microwave plasma ionization mass spectrometry system that enables MS analysis with high coverage.
- Fengjian Chu
- , Gaosheng Zhao
- & Xiaozhi Wang
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Article
| Open AccessDemethylation C–C coupling reaction facilitated by the repulsive Coulomb force between two cations
Carbon chain elongation (CCE) is normally carried out using either chemical catalysts or bioenzymes. Herein we demonstrate a catalyst-free approach to promote demethylation C–C coupling reactions for advanced CCE constructed with functional groups under ambient conditions.
- Xiaoping Zhang
- , Keke Huang
- & Huanwen Chen
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Article
| Open AccessOverhauser enhanced liquid state nuclear magnetic resonance spectroscopy in one and two dimensions
The authors report signal enhancements in high-resolution liquid-state NMR by a new setup for dynamic nuclear polarization. Two-dimensional NMR techniques are used to transfer hyperpolarization within the nuclei of molecules such as metabolites or drugs.
- Marcel Levien
- , Luming Yang
- & Marina Bennati
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| Open AccessGlobal protein turnover quantification in Escherichia coli reveals cytoplasmic recycling under nitrogen limitation
Gupta, Johnson et al. quantify the turnover rates of ~3200 E. coli proteins, demonstrating that cytoplasmic proteins are recycled when nitrogen is limited and that protein degradation rates are generally uncoupled from cell division rates.
- Meera Gupta
- , Alex N. T. Johnson
- & Martin Wühr
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Article
| Open AccessWhite-light activatable organic NIR-II luminescence nanomaterials for imaging-guided surgery
Second near-infrared (NIR-II) fluorescence imaging is promising for real-time surveillance of surgical operations, but its clinical uses have been limited by the safety and cost concerns associated with lasers or X-rays. Here the authors report the engineering and applications of white-light activatable organic nanomaterials with bright NIR-II emission.
- Chunbin Li
- , Jian Du
- & Ben Zhong Tang
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Article
| Open AccessHigh throughput platform technology for rapid target identification in personalized phage therapy
Phage therapy often relies on labour-intensive and time-consuming methods that could lead to delays in medical treatment. Here, authors describe an all-in-one solution for navigating multiple, large, decentralized biobanks, allowing for rapid high-throughput phage susceptibility testing.
- Fereshteh Bayat
- , Arwa Hilal
- & Zeinab Hosseinidoust
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Article
| Open AccessRadially distributed charging time constants at an electrode-solution interface
Classical theories of electrode kinetics assume a homogeneous electrode-solution interface. Here, authors reveal that electron transfer at a macroscopic electrode exhibits significant spatial inhomogeneity due to nonuniform solution resistance, which can be reduced by a retracted electrode design.
- Ben Niu
- , Ruo-Chen Xie
- & Wei Wang
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Article
| Open AccessIlluminating the dark space of neutral glycosphingolipidome by selective enrichment and profiling at multi-structural levels
The molecular profiling of glycosphingolipids (GSLs) is hindered by the coexistence of abundant phospholipids and diverse isomers. The authors introduce a highly sensitive workflow that maps out the structural atlas of neutral GSLs, previously deemed a “dark space” within the lipidome.
- Zidan Wang
- , Donghui Zhang
- & Yu Xia
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Article
| Open AccessBarbed arrow-like structure membrane with ultra-high rectification coefficient enables ultra-fast, highly-sensitive lateral-flow assay of cTnI
Acute myocardial infarction has become a public health disease threatening public life safety. Here, authors propose a BAS Mem with an ultra-high rectification coefficient, replacing the conventional chromatographic membrane to develop an ultra-fast, highly-sensitive lateral-flow assay for cTnI.
- Juanhua Li
- , Yiren Liu
- & Jianhua Zhou
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Article
| Open Access200 GHz single chip microsystems for dynamic nuclear polarization enhanced NMR spectroscopy
Cutting the cost and complexity of the microwave devices is crucial for expanding the applications of DNP enhanced NMR. Researchers introduce microsystems where the generation/detection of 200 GHz microwaves occur locally on a 1 mm2 silicon chip.
- Nergiz Sahin Solmaz
- , Reza Farsi
- & Giovanni Boero
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Article
| Open AccessCharacterize direct protein interactions with enrichable, cleavable and latent bioreactive unnatural amino acids
The high-throughput identification of cross-linking peptides is challenging. Here, the authors developed an enrichable and cleavable latent bioreactive unnatural amino acid eFSY, and a software AixUaa to improve the cross-linking peptides indentification in live cells.
- Dan-Dan Liu
- , Wenlong Ding
- & Bing Yang
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Article
| Open AccessMechanistic understanding of speciated oxide growth in high entropy alloys
Understanding the intricate relationship between alloying elements and oxidation processes is essential for the integrity and performance of materials. Here, the authors study the effects of atomic size and redox potential to understand the oxidation process and structural changes in surface oxides.
- Bharat Gwalani
- , Andrew Martin
- & Arun Devaraj
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Article
| Open AccessEvolution of the ionisation energy with the stepwise growth of chiral clusters of [4]helicene
Polycyclic aromatic hydrocarbons such as [4]helicenes are important interstellar molecules. Here, the authors show their evolution of chiral clusters upon aggregation through coincidence spectroscopy and quantum chemical calculations.
- Sérgio R. Domingos
- , Denis S. Tikhonov
- & Melanie Schnell
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Article
| Open AccessA spatially localized DNA linear classifier for cancer diagnosis
Molecular computing is an emerging paradigm with a crucial role in clinical diagnosis. Here, authors develop a spatially localized, DNA-integrated circuits-based classifier, DNA IC-CLA, which enables accurate cancer diagnosis for clinical samples in a faster and more effective manner.
- Linlin Yang
- , Qian Tang
- & Da Han
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Article
| Open AccessZero-field J-spectroscopy of quadrupolar nuclei
Zero to ultralow-field NMR provides chemical information in the absence of a high magnetic field but it is difficult to measure molecules with quadrupolar nuclei due to their fast relaxation. This study examines zero-field J-spectra from isotopologues of ammonium cations, with quadrupolar nuclei, revealing the presence of a primary isotope effect of −58 mHz.
- Román Picazo-Frutos
- , Kirill F. Sheberstov
- & Danila A. Barskiy
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Article
| Open AccessTimescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides
Differences in timescales of electron transfer reactions limit the efficiency of electrochemiluminescence. Here, the authors coordinate the timescales using shallow trap states in carbon nitride to achieve high efficiencies applied in nitrite sensing.
- Yanfeng Fang
- , Hong Yang
- & Yuanjian Zhang
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Article
| 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