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science Bulletin 2024年第2期69卷 159-162页

作者： Si-Yuan Yu Yi-Li Liu Zheng Li Dechen Jiang Jing-Juan Xu Hong-Yuan Chen Wei-Wei Zhao state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1.3].However,despite their importance,current nanoelectrode preparations are highly restrained to flame/electrochemical etching,metal sputtering,electrochemical deposition,etc.[3],resulting in a limited range of materials(mainly gold,platinum and carbon)for potential-resolved detection of redox-active species(Table S1.online).The enrichment of preparation methods to introduce novel materials and mechanisms should prove significant for the development of nanoelectrodes.

关键词： electrode deepening restrained

Selective and asymmetric ion transport in covalent organic framework-based two-dimensional nanofluidic devices

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International Journal of Smart and Nano Materials 2024年第1期15卷 186-197页

作者： Li-Qiu Huang Shuang Chen Ri-Jian Mo Zhong-Qiu Li Xing-Hua Xia state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjingChina

Two-dimensional(2D)covalent organic framework(COF)mem-branes featuring well-aligned and programmable vertical nano-channels have emerged as a promising candidate for advanced nanofluidic devices and showcased vast potential in the fields of smart-gating,ion-separation,and ***,the transverse interlayer nanochannels with a height of sub-nanometer-scale in 2D-COF membranes have scarcely been studied in ***,we report the ion transport characteristics in 2D interlayer nanochannels of protonated CoF *** dis-tinct surface-charge-governed ionic conductance in domination of electrolyte concentration below 1.-3 M as well as the exceptional anion/cation(Cl^(-)/K^(+))selectivity is revealed due to the pronounced charge and nano-confinement ***,evident ion current rectification is witnessed when incorporating asymmetric geometry into the system,which is attributed to the dynamic process of ion enrichment and dissipation within the protonated *** work offers immense prospects for 2D-COF membranes in the fields of biomimetic nanofluidic devices and cutting-edge electronic devices.

关键词： Two-dimensional covalent organic framework interlayernanochannels ion transport characteristics nanofluidic device

Atomic force microscopy-based nanoscale infrared techniques for liquid environments

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science Bulletin 2024年第2期69卷 151-153页

作者： Jian Li Jing Liang Mu-Hao Lan Xing-Hua Xia state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Infrared(IR)light energy matches well with the vibration and rotation of chemical bonds in molecules,hence IR spectroscopy is commonly used for accurate molecular identification[1..Conventional IR analysis involves bulk samples,providing averaged information of the entire *** spatially-resolved investigation of heterogeneous sample properties is constrained by the micrometer-level spatial resolution of optical IR microscopy.

关键词： spatially hence rotation

Photoredox-catalyzed C-glycosylation of peptides with glycosyl bromides

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Chinese Chemical Letters 2024年第6期35卷 263-267页

作者： Chen Li Ziyuan Zhao Shouyun Yu state {1. laboratory of analytical chemistry for life science Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Glycosyl radicals,produced under mild photoredox conditions,show unique utility in the preparation of C-linked *** herein report the construction of C-glycosidic bonds on α,β-dehydroalanine(DHA)of peptides with easily available glycosyl bromides as glycosyl radical precursors under highly anomeric control,leading to C-glycosylation modifications of *** method not only has outstanding functional group compatibility,but also is feasible in near-physiological conditions(pH~7 and temperature T≤37℃ in aqueous media).

关键词： Glycosylation C-Glycosides Glycopeptides Dehydroalanine Photoredox catalysis

Dynamic Measurement of Intracellular pH Based on Bioluminescent Bacteria

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Chemical Research in Chinese Universities 2024年第2期40卷 287-292页

作者： LI Yaohua WANG Wei state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringChemBIC(Chemistry and Biomedicine Innovation Center)Nanjing UniversityNanjing210023P.R.China

Intracellular pH(pHi)is a fundamental indicator of cellular physiological state,regulating cellular state and function,and has important research *** various probes for measuring intracellular pH were available,it is challenging to reflect pHi in real-time and reversible ***,we developed a whole-cell bioluminescent(BL)probe based on wild type BL bacteria,photobacterium phosphoreum(***),to determine and image *** dependence of BL intensity of *** on pH values of culture solutions was *** was found that BL intensity could respond to the change of pH values rapidly and *** further revealed that *** maintained pH homeostasis in the extracellular pH(pHe)within the range of 5.0–7.0,while intracellular pH homeostasis was destroyed at the alkaline *** method opens up the enormous potential of BL bacteria as an alternative to fluorescence for monitoring and imaging pHi.

关键词： Bioluminescence P.phosphoreum Intracellular pH Cell imaging

Reversibly Tuning Electrochemiluminescence with Stimulated Emission Route for Single-Cell Imaging

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Research 2024年第3期2023卷 205-215页

作者： Cheng Ma Xiaodan Gou Zejing Xing Min-Xuan Wang Wenlei Zhu Qin Xu Dechen Jiang Jun-Jie Zhu School of chemistry and Chemical Engineering Yangzhou University.Yangzhou 225002P.R.China state {1. laboratory of analytical chemistry for life science State Key Laboratory of Pollution Control and Resource ReuseSchool of Chemistry and Chemical EngineeringSchool of the EnvironmentNanjing UniversityNanjing 210023P.R.China.

Electrochemiluminescence (ECL) has established itself as an excellent transduction technique in biosensing and light-emitting device, while conventional ECL mechanism depending on spontaneous emission of luminophores lacks reversibility and tunable emission characters, limiting the universality of ECL technique in the fields of fundamental research and clinical applications. Here, we report the first observation of stimulated emission route in ECL and thus establish a reversible tuning ECL microscopy for single-cell imaging. This microscopy uses a focused red-shifted beam to transfer spontaneous ECL into stimulated ECL, which enables selective and reversible tuning of ECL emission from homogeneous solution, single particles, and single cells. After excluding other possible competitive routes, the stimulated ECL emission route is confirmed by a dual-objective system in which the suppressed spontaneous ECL is accompanied by the enhanced stimulated ECL. By incorporating a commercial donut-shaped beam, the sharpness of single-cell matrix adhesion is improved 2 to 3 times compared with the counterpart in confocal ECL mode. The successful establishment of this stimulated emission ECL will greatly advance the development of light-emitting device and super-resolution ECL microscopy.

关键词： tuning beam limiting

Cationic Conjugated Oligomers for Efficient and Rapid Antibacterial Photodynamic Therapy via Both Type Ⅰ and Type Ⅱ Pathways

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Chinese Journal of chemistry 2024年第1期42卷 61-66页

作者： Huan Wang Shuwen Guo Qiong Yuan Meiqi Li Yanli Tang Country key {1. of analytical chemistry for life science of Shaanxi Province Key Laboratory of Applied Surface and Colloid ChemistryMinistry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'anShaanxi 710119China

Recently,photodynamic therapy(PDT)has attracted wide attention due to its less susceptibility to drug resistance,broad-spectrum biocidal activity and biosafety in normal ***,the traditional photosensitizers(Ps)face the disadvantage of poor therapeutic efficacy due to the requirement of an aerobic environment to generate ^(1.O_(2) through Type Ⅱ ***,we designed and synthesized a novel cationic conjugated oligomer oligo(phenylene vinylene)(OPV)and studied its antibacterial photodynamic activity against both Gram-negative Escherichia coli(***)and Gram-positive bacteria methicillin-resistant Staphylococcus aureus(MRSA).Importantly,the OpV can rapidly produce reactive oxygen species(ROs)through double pathways,Type Ⅰ and Ⅱ mechanism under white light irradiation,and efficiently kill *** and MRSA at a nanomolar *** dual type photosensitizing capability makes OPV promising for enhanced PDT to treat pathogens and tumors in complex environments.

关键词： Conjugated oligomers Antibacterial photodynamic therapy Oligo(phenylene vinylene) Reactive oxygen species Typelandll pathways

In Vivo Voltammetric Imaging of Metal Nanoparticle-Catalyzed Single-Cell Electron Transfer by Fermi Level-Responsive Graphene

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Research 2024年第1期2023卷 271-280页

作者： Qing Xia Rui Liu Xueqin Chen Zixuan Chen Jun-Jie Zhu state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023P.R.China Shenzhen Research Institute of Nanjing University Shenzhen 518000P.R.China

Metal nanomaterials can facilitate microbial extracellular electron transfer(EET)in the electrochemically active ***,the role of nanomaterials/bacteria interaction in this process is still ***,we reported the single-cell voltammetric imaging of Shewanella oneidensis MR-1.at the single-cell level to elucidate the metal-enhanced EET mechanism in vivo by the Fermi level-responsive graphene *** oxidation currents of~20 fA were observed from single native cells and gold nanoparticle(AuNP)-coated cells in linear sweep voltammetry *** the contrary,the oxidation potential was reduced by up to 1.0 mV after AuNP *** revealed the mechanism of AuNP-catalyzed direct EET decreasing the oxidation barrier between the outer membrane cytochromes and the *** method offered a promising strategy to understand the nanomaterials/bacteria interaction and guide the rational construction of EET-related microbial fuel cells.

关键词： Fermi voltammetry Electron

Controllable CPL response driven by achiral UV-photosensitive dichroic dye through cholesteric liquid crystals

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science China {1. 2024年第4期67卷 1250-1255页

作者： Yihan Chen Yang Li Hang Li Lulu Li Yiwu Quan Yixiang Cheng state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China key {1. of High-Performance Polymer Material and Technology of Ministry of Education School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Versatile stimuli-responsive circularly polarized luminescent(CPL)materials have potential applications in information storage,security encryption,and intelligent *** this study,the Z/E isomerization of ultraviolet(UV)-photosensitive achiralα-cyanostilbene derivative was used as an achiral dichroic dye(Switch)to drive the controllable CPL-active response in cholesteric liquid crystals(CLCs).Under irradiation by 365 nm UV light,the resulting CLCs-Z-Switch underwent a Z-to-E configuration isomerization as CLCs-E-Switch,accompanied by a decrease in its dichroic order parameter(SFvalue)from 0.1.to *** the quantum yield(QY)of CLCs-E-Switch increased from 8.1.(CLCs-Z-Switch)to 1..8%,the corresponding glumvalues of CPL emission decreased from+0.55/-0.57 to+0.37/-0.39 due to a decrease in the order of helical arrangement of E-Switch in E7 *** study enables photosensitive CLCs-Switch to be applied for optical information storage devices.

关键词： circularly polarized luminescent photosensitive dichroic dye cholesteric liquid crystals chiral induction

Aggregation-induced delayed electrochemiluminescence of organic dots in aqueous media

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Aggregate 2024年第1期5卷 167-174页

作者： Hang Gao Shen-Yu Shi Shu-MinWang Qian-Qian Tao Hui-Li Ma Jun Hu Hong-Yuan Chen Jing-Juan Xu state {1. laboratory of analytical chemistry for life science School of Chemistry and Chemical EngineeringNanjing UniversityNanjingChina key {1. of Flexible Electronics(KLOFE)and Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjingChina School of life {1. and Health Engineering Jiangnan UniversityWuxiChina

Full utilization of the excited species at both singlet states(1.*)and triplet states(3R*)is crucial to improving electrochemiluminescence(ECL)efficiency but is challenging for organic luminescent ***,an aggregation-induced delayed ECL(AIDECL)active organic dot(OD)containing a benzophenone acceptor and dimethylacridine donor is reported,which shows high ECL efficiency via reverse intersystem crossing(RISC)of non-emissive 3R*to emissive 1.*,overcoming the spin-forbidden radiative decay from 3R*.By introducing dual donor-acceptor pairs into luminophores,it is found that nonradiative pathway could be further suppressed via enhanced intermolecular weak interactions,and multiple spin-up conversion channels could be *** a consequence,the obtained OD enjoys a 6.8-fold higher ECL efficiency relative to the control AIDECL-active ***-crystal studies and theoretical calculations reveal that the enhanced AIDECL behaviors come from the acceleration of both radiative transition and *** work represents a major step towards purely organic,high-efficiency ECL dyes and a direction for the design of next-generation ECL dyes at the molecular level.

关键词： aggregation-induced delayed electrochemiluminescence benzophenone dimethylacridine organic dots reverse intersystem crossing