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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology institute of Sustainability for Chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of Materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Activation energy

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Activating weak electrophiles to break nonpolar C-C bonds with electric fields

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Chinese Chemical Letters 2023年第11期34卷 1-2页

作者： Xueyan Zhao Adila Adijiang Dong Xiang institute of Modern Optics and Center of single-Molecule Science Tianjin Key Laboratory of Micro-scale Optical Information Science and TechnologyNankai UniversityTianjin 300350China School of Materials Science and Engineering Smart Sensing Interdisciplinary Science CenterNankai UniversityTianjin 300350China

Electrophilic aromatic substitution(EAS)is a vital chemical reaction in organic chemistry that involves replacing substituent on an aromatic ring by an *** its widespread industrial applications in the production of substituted aromatic compounds,the reaction typically requires harsh reaction conditions,such as high temperature and potent Lewis acid catalysts,to activate the electrophile due to the stability of the aromatic ring[1].Recently,a study published by Yaping Zang and colleagues in Nature Communications demonstrates the use of an electric field as a catalyst to regulate EAS reactivity,replacing conventional chemical *** research team discovered that an electric field could activate an otherwise unreactive electrophile and break inert nonpolar C-C bonds under mild *** unprecedented results showcase the potential for broadening the scope of EAS reactions via electric field catalysis.

关键词： bonds aromatic polar

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Integrated proteomic and phosphoproteomic data-independent acquisition data evaluate the personalized drug responses of primary and metastatic tumors in colorectal cancer

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Biophysics Reports 2023年第2期9卷 67-81页

作者： Xumiao Li Yiming Huang Kuo Zheng Guanyu Yu Qinqin Wang Lei Gu Jingquan Li Hui Wang Wei Zhang Yidi Sun Chen Li Center for single-Cell Omics School of Public Health Shanghai Jiao Tong University School of Medicine institute of Neuroscience CAS Center for Excellence in Brain Science and Intelligence Technology Chinese Academy of Sciences Colorectal Surgery Department Changhai Hospital Naval Medical University

Mass spectrometry(MS)-based proteomics and phosphoproteomics are powerful methods to study the biological mechanisms, diagnostic biomarkers, prognostic analysis, and drug therapy of tumors. Dataindependent acquisition(DIA) mode is considered to perform better than data-dependent acquisition(DDA) mode in terms of quantitative reproducibility, specificity, accuracy, and identification of low-abundance proteins. Mini patient derived xenograft(Mini PDX) model is an effective model to assess the response to antineoplastic drugs in vivo and is helpful for the precise treatment of cancer *** are favorable spots for tumor-targeted drugs, and their functional completion relies on signaling pathways through phosphorylating downstream substrates. Kinase-phosphorylation networks or edge interactions are considered more credible and permanent for characterizing complex ***, we provide a workflow for personalized drug response assessment in primary and metastatic colorectal cancer(CRC) tumors using DIA proteomic data, DIA phosphoproteomic data, and Mini PDX models. Three kinase inhibitors, afatinib, gefitinib, and regorafenib, are tested pharmacologically. The process mainly includes the following steps: clinical tissue collection, sample preparation, hybrid spectral libraries establishment, MS data acquisition, kinase-substrate network construction, in vivo drug test, and elastic regression modeling. Our protocol gives a more direct data basis for individual drug responses, and will improve the selection of treatment strategies for patients without the druggable mutation.

关键词： Proteomics Phosphoproteomics Data-independent acquisition (DIA) Mini patient derived xenograft (MiniPDX) Kinase-substrate network Personalized drug responses

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single-cell technologies: current and near future

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Science China Life Sciences 2025年第01期 1-4页

作者： Chenfei Wang Qi Liu Xiaohui Fan Tieliu Shi Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration Ministry of EducationOrthopedics DepartmentTongji HospitalBioinformatics DepartmentSchool of Life Sciences and TechnologyTongji University Frontier Science Center for Stem Cells School of Life Sciences and TechnologyTongji University Translational Medical Center for Stem Cell Therapy and institute for Regenerative Medicine Shanghai East HospitalBioinformatics DepartmentSchool of Life Sciences and TechnologyTongji University Research institute of Intelligent Computing Zhejiang Lab Pharmaceutical Informatics institute College of Pharmaceutical SciencesZhejiang University National Key Laboratory of Chinese Medicine Modernization Innovation Center of Yangtze River DeltaZhejiang University Center for Bioinformatics and Computational Biology Shanghai Key Laboratory of Regulatory Biologythe Institute of Biomedical Sciences and School of Life SciencesEast China Normal University Key Laboratory of Advanced Theory and Application in Statistics and Data Science (MOE) School of StatisticsEast China Normal University

single-cell technologies enable the indepth exploration of multiple biological hierarchies at the scale of individual cells,which have deepened our knowledge of cellular diversity, tissue organization, and overall organism function(Sun et al.,2024). In 2009, single-cell RNA sequencing(sc RNA-seq) was first developed as a powerful tool to dissect gene expression and uncover transcriptional *** the rapid advancement of technology, single-cell approaches have expanded to encompass other omics, such as genomics, epigenomics, proteomics,and metabolomics.

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Bimetallic single‑Atom Catalysts for Water Splitting

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Nano-Micro Letters 2025年第1期17卷 1-45页

作者： Megha A.Deshmukh Aristides Bakandritsos Radek Zbořil Nanotechnology Centre Centre for Energy and Environmental TechnologiesVŠB–Technical University of Ostrava17.listopadu 2172/1570800 Ostrava‑PorubaCzech Republic Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute(CATRIN)Palacky University OlomoucŠlechtitelů241/2778371 Olomouc–HoliceCzech Republic

Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead the global transition to a fossil fuel-independent *** field of catalysis has been revolutionized by single-atom catalysts(SACs),which exhibit unique and intricate interactions between atomically dispersed metal atoms and their ***,bimetallic SACs(bimSACs)have garnered significant attention for leveraging the synergistic functions of two metal ions coordinated on appropriately designed *** offer an avenue for rich metal–metal and metal–support cooperativity,potentially addressing current limitations of SACs in effectively furnishing transformations which involve synchronous proton–electron exchanges,substrate activation with reversible redox cycles,simultaneous multi-electron transfer,regulation of spin states,tuning of electronic properties,and cyclic transition states with low activation *** review aims to encapsulate the growing advancements in bimSACs,with an emphasis on their pivotal role in hydrogen generation via water *** subsequently delve into advanced experimental methodologies for the elaborate characterization of SACs,elucidate their electronic properties,and discuss their local coordination ***,we present comprehensive discussion on the deployment of bimSACs in both hydrogen evolution reaction and oxygen evolution reaction,the two half-reactions of the water electrolysis process.

关键词： single-atom catalysts single-atom dimers Hydrogen evolution Oxygen evolution Water splitting

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High Fe‑Loading single‑Atom Catalyst Boosts ROS Production by Density Effect for Efficient Antibacterial Therapy

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Nano-Micro Letters 2025年第2期17卷 187-203页

作者： Si Chen Fang Huang Lijie Mao Zhimin Zhang Han Lin Qixin Yan Xiangyu Lu Jianlin Shi Department of Cardiology Shanghai Tenth People’s HospitalSchool of MedicineTongji UniversityShanghai 200092People’s Republic of China Shanghai institute of Ceramics Chinese Academy of SciencesShanghai 200050People’s Republic of China Shanghai Frontiers Science Center of Nanocatalytic Medicine School of MedicineTongji UniversityShanghai 200092People’s Republic of China

The current single-atom catalysts(SACs)for medicine still suffer from the limited active site ***,we develop a synthetic method capable of increasing both the metal loading and mass-specific activity of SACs by exchanging zinc with *** constructed iron SACs(h^(3)-FNC)with a high metal loading of 6.27 wt%and an optimized adjacent Fe distance of~4 A exhibit excellent oxidase-like catalytic performance without significant activity decay after being stored for six months and promising antibacterial ***,a“density effect”has been found at a high-enough metal doping amount,at which individual active sites become close enough to interact with each other and alter the electronic structure,resulting in significantly boosted intrinsic activity of single-atomic iron sites in h^(3)-FNCs by 2.3 times compared to low-and medium-loading ***,the overall catalytic activity of h^(3)-FNC is highly improved,with mass activity and metal mass-specific activity that are,respectively,66 and 315 times higher than those of commercial Pt/*** addition,h^(3)-FNCs demonstrate efficiently enhanced capability in catalyzing oxygen reduction into superoxide anion(O_(2)·^(−))and glutathione(GSH)*** in vitro and in vivo assays demonstrate the superior antibacterial efficacy of h^(3)-FNCs in promoting wound *** work presents an intriguing activity-enhancement effect in catalysts and exhibits impressive therapeutic efficacy in combating bacterial infections.

关键词： Nanocatalytic medicine single-atom catalysts Reactive oxygen species(ROS) High metal loading Oxidase catalysis

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A high-performance molecular switch fabricated by the two-dimensional van der Waals heterojunction

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National Science Review 2023年第7期10卷 73-74页

作者： Xubin Zhang Adila Adijiang Dong Xiang institute of Modern Optics and Center of single-Molecule Science Tianjin Key Laboratory of Micro-scale Optical Information Science and Technology Nankai University Tong Lu Fei Ran Garment-Nankai University Joint Laboratory Nankai University School of Materials Science and Engineering Smart Sensing Interdisciplinary Science Center Nankai University

Since the concept that single molecules can be used as electronic components to construct active electronic devices was proposed,the preparation of commercially available single-molecule switches has become a research *** break through the dilemma of electronic components facing the failure of Moore’s Law and further reduce the size of a chip,developing single-molecule electronics is particularly important and has yielded a wealth of *** research groups have successfully used optical fields[1,2],electric fields [3-5],and electrochemical methods [6] to modulate single-molecule behaviors and achieve single-molecule switching properties.

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single-molecule conductance measurements reveal a new catalytic mechanism of formate dehydrogenase

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Science China Chemistry 2023年第8期66卷 2163-2165页

作者： Shichao Zhong Zhiheng Yang Xuefeng Guo Beijing National Laboratory for Molecular Sciences National Biomedical Imaging CentreCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Centre of single-Molecule Sciences Institute of Modern OpticsFrontiers Science Centre for New Organic MatterCollege of Electronic Information and Optical EngineeringNankai UniversityTianjin300350China

Elucidating the functional mechanism of biological enzyme functions is always an important topic in biochemistry because of its great importance for understanding life activities and developing potential ***,ensemble methods commonly used in the analysis of enzyme kinetics can only provide average information on a large number of molecules.

关键词： mechanism kinetics conductance

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Genome-wide adenine N6-methylation map reveals epigenomic regulation of lipid accumulation in Nannochloropsis

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Plant Communications 2024年第3期5卷 106-122页

作者： Yanhai Gong Qintao Wang Li Wei Wensi Liang Lianhong Wang Nana Lv Xuefeng Du Jiashun Zhang Chen Shen Yi Xin Luyang Sun Jian Xu single-Cell Center CAS Key Laboratory of BiofuelsShandong Key Laboratory of Energy GeneticsQingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdaoChina Shandong Energy institute QingdaoChina Qingdao New Energy Shandong Laboratory QingdaoChina University of Chinese Academy of Sciences Beijing 100049China Laboratory for Marine Biology and Biotechnology Qingdao National Laboratory for Marine Science and TechnologyQingdao 266237China

Epigenetic marks on histones and DNA,such as DNA methylation at N6-adenine(6mA),play crucial roles in gene expression and genome maintenance,but their deposition and function in microalgae remain largely ***,we report a genome-wide 6mA map for the model industrial oleaginous microalga Nannochloropsis oceanica produced by single-molecule real-time *** in 0.1%of adenines,6mA sites are mostly enriched at the AGGYV motif,more abundant in transposons and 30 untranslated re-gions,and associated with active ***,6mA gradually increases in abundance along the direction of gene transcription and shows special positional enrichment near splicing donor and transcrip-tion termination *** expressed genes tend to show greater 6mA abundance in the gene body than do poorly expressed genes,indicating a positive interaction between 6mA and general transcription ***,knockout of the putative 6mA methylase NO08G00280 by genome editing leads to changes in methylation patterns that are correlated with changes in the expression of molybdenum cofactor,sulfate transporter,glycosyl transferase,and lipase genes that underlie reductions in biomass and oil *** contrast,knockout of the candidate demethylase NO06G02500 results in increased 6mA levels and reduced *** the epigenomic players and their roles in biomass productivity and lipid metabolism lays a foundation for epigenetic engineering of industrial microalgae.

关键词： adenine N6-methylation industrial oleaginous microalgae Nannochloropsis oceanica transcriptional regulation epigenomics

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Structural Transition Dynamics in Carbon Electrode-Based single-Molecule Junctions

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Chinese Journal of Chemistry 2021年第2期39卷 223-231页

作者： Peihui Li Chuancheng Jia Xuefeng Guo Center of single-Molecule Sciences Institute of Modern OpticsCollege of Electronic Information and Optical EngineeringNankai University38 Tongyan RoadJinnan DistrictTianjin300350 China Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871 China

Monitoring the structural transitions of individual molecules is of great significance because it helps to in depth explore the properties of molecules and provide diverse possibilities for molecular applications in the fields of chemistry,biology and material *** review summarizes the strategy of using single-molecule electrical approaches to study molecular structure transitions at the single-molecule level in real ***,through the use of stable single-molecule devices for real-time electrical monitoring,the process of molecular structure transitions of a single molecule can be investigated,which helps to explore the nature of molecules in chemical and biological *** particular,the detection methods have been extended to the investigation of biological macromolecules for monitoring the conformational changes of nucleotide chains in different systems,such as double helix DNA,aptamer and DNA *** the end,we discuss the future challenges of probing structural transitions of single molecules,and provide prospects for further breakthroughs in this field.

关键词： Structural transition Photoisomerism Molecular electronics Noncovalent interactions Stereoelectronic effect

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