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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 key 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 100 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

In-situ synthesis of quantum dots in the nucleus of live cells

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National Science Review 2024年第3期11卷 172-182页

作者： Yusi Hu Zhi-Gang Wang Haohao Fu Chuanzheng Zhou Wensheng Cai Xueguang Shao Shu-Lin Liu Dai-Wen Pang state key laboratory of Medicinal Chemical Biology Frontiers Science Centre for New Organic MatterTianjin Key Laboratory of Biosensing and Molecular Recognition Research Centre for Analytical Sciences College of Chemistry School of Medicine and Frontiers Science Centre for Cell Responses Nankai University Haihe laboratory of Sustainable Chemical Transformations

The cell nucleus is the main site for the storage and replication of genetic material, and the synthesis of substances in the nucleus is rhythmic, regular and strictly regulated by physiological processes. However,whether exogenous substances, such as nanoparticles, can be synthesized in situ in the nucleus of live cells has not been reported. Here, we have achieved in-situ synthesis of CdSxSe1-xquantum dots（QDs） in the nucleus by regulation of the glutathione（GSH） metabolic pathway. High enrichment of GSH in the nucleus can be accomplished by the addition of GSH with the help of the Bcl-2 protein. Then, high-valence Se is reduced to low-valence Se by glutathione-reductase-catalyzed GSH, and interacts with the Cd precursor formed through Cd and thiol-rich proteins, eventually generating QDs in the nucleus. Our work contributes to a new understanding of the syntheses of substances in the cell nucleus and will pave the way for the development of advanced ‘supercells’.

关键词： glutathione live cell nucleus quantum dot intracellular synthesis

CoFe_(2)O_(4) decorated graphene/C_(18)-functionalized mesoporous silica nanocomposites prepared for magnetic enrichment and electrochemical detection of promethazine in beef

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Chinese Chemical Letters 2024年第3期35卷 208-213页

作者： Xingdong Yang Shi-Ming Ying Sen Zhang Jinxia Dai Wei Gao Tian-Qi Wang Jun-Qin Qiao Hong-Zhen Lian Li Mao state key laboratory of analytical chemistry for Life Science School of Chemistry&Chemical Engineering and Centre of Materials AnalysisNanjing UniversityNanjing 210023China Ministry of Education(MOE)key laboratory of Modern Toxicology School of Public HealthNanjing Medical UniversityNanjing 211166China

Promethazine(PHZ)is used as a sedative in veterinary medicine,and its residue can threaten the health of *** electrochemical detection of PHZ is suitable method for application in the ***,the traditional electroanalysis is difficult to perform directly in meat samples due to matrix *** work integrates magnetic solid-phase extraction and differential pulse voltammetry for highly sensitive and selective determination of PHZ in beef and beef liver for the first ***_(2)O_(4)/graphene coated with C_(18)-functionalized mesoporous silica(MG@mSiO_(2)-C_(18))is synthesized as dispersed magnetic adsorbent to extract *** glassy carbon electrode modified with nitrogen-doped hollow carbon microspheres(HCM)attracts the MG@mSiO_(2)-C_(18)with PHZ,and directly detects the PHZ without elution ***@mSiO_(2)-C_(18)can separate PHZ to avoid the interference of impurities on following detection,and also concentrate PHZ on magnetic ***,the electrode modification with HCM can amplify the electrochemical signal of ***,the integrated PHZ determination method exhibits a wide linear range from 0.08μmol/L to 300μmol/L with a low limit of detection of 9.8 nmol/*** beef sample analysis presents excellent recovery,demonstrating that this protocol is promising for the rapid and onsite detection of PHZ in real meat samples。

关键词： Promethazine(PHZ) Drug residue Magnetic solid phase extraction Electrochemical detection Beef

Rapid and controllable in-situ self-assembly of main-group metal nanofilms for highly efficient CO_(2)electroreduction to liquid fuel in flow cells

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Nano Research 2024年第6期17卷 5718-5725页

作者： Miao Wang Huaizhu Wang Yaoda Wang Junchuan Liang Mengfei Zhu Jiarui Li Zuoxiu Tie Zhong Jin state key laboratory of Coordination chemistry MOE Key Laboratory of Mesoscopic ChemistryMOE Key Laboratory of High Performance Polymer Materials and TechnologyJiangsu Key Laboratory of Advanced Organic MaterialsTianchang New Materials and Energy Technology Researc

The electrocatalytic reduction of CO_(2)is a promising pathway to generate renewable fuels and ***,its advancement is impeded by the absence of electrocatalysts with both high selectivity and ***,we present a scalable in-situ thermal evaporation technique for synthesizing series of Bi,In,and Sn nanofilms on carbon felt(CF)substrates with a high-aspect-ratio *** resulting main-group metal nanofilms exhibit a homogeneously distributed and highly exposed catalyst surface with ample active sites,thereby promoting mass transport and ad-/desorption of reaction *** from the unique fractal morphology,the Bi nanofilms deposited on CF exhibit optimal catalytic activities for CO_(2)electroreduction among the designed metal nanofilms electrodes,with the highest Faradaic efficiency of 96.9%for formate production at−1.3 V *** hydrogen electrode(RHE)in *** an industrially relevant current density of 221.4 mA·cm−2 in flow cells,the Bi nanofilms retain a high Faradaic efficiency of 81.7%at−1.1 V(***)and a good long-term stability for formate ***,a techno-economic analysis(TEA)model shows the potential commercial viability of electrocatalytic CO_(2)conversion into formate using the Bi nanofilms *** results offer a green and convenient approach for in-situ fabrication of stable and inexpensive thin-film catalysts with a fractal structure applicable to various industrial settings.

关键词： CO_(2)electroreduction non-noble metal nanofilms flow cells efficiency and selectivity techno-economic analysis

Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China chemistry 2024年第6期67卷 1935-1940页

作者： Ya-Ping Shao Zhuo-Min Chi Yong-Min Liang state key laboratory of Applied Organic chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor *** method enables the synthesis of diverseβ-orγ-branched aromatic *** mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable ***,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

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Electrochemical synthesis of trimetallic nickel-iron-copper nanoparticles via potential-cycling for high current density anion exchange membrane water-splitting applications

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Journal of Energy chemistry 2024年第2期89卷 535-542,I0012页

作者： Ziqi Zhang Sheng Wan Hanbo Wang Jinghan He Ruige Zhang Yuhang Qi Haiyan Lu state key laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012JilinChina

Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil *** water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity ***,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment ***,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel *** synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline ***,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.

关键词： Electrocatalytic water splitting Hydrogen evolution reaction Oxygen evolution reaction Electrochemical synthesis Anion exchange membrane

Integration of morphology and electronic structure modulation on cobalt phosphide nanosheets to boost photocatalytic hydrogen evolution from ammonia borane hydrolysis

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Green Energy & Environment 2024年第2期9卷 333-343页

作者： Chao Wan Yu Liang Liu Zhou Jindou Huang Jiapei Wang Fengqiu Chen Xiaoli Zhan Dang-guo Cheng School of chemistry and Chemical Engineering Anhui Province Key Laboratory of Coal Clean Conversion and High Valued UtilizationAnhui University of TechnologyMa'anshan243002China College of Chemical and Biological Engineering Zhejiang UniversityZhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology38 Zheda RoadHangzhou310027China key laboratory of New Energy and Rare Earth Resource Utilization of state ethnic affairs commission Key Laboratory of Photosensitive Materials&Devices of Liaoning ProvinceSchool of Physics and Materials EngineeringDalian Nationalities University 18 Liaohe West RoadDalian116600China Institute of Zhejiang University-Quzhou 78 Jiuhua Boulevard NorthQuzhou324000China Jiangsu key laboratory of Advanced Catalytic Materials and Technology Changzhou University213164China

The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen *** borane(AB)has regarded as a competitive candidate for chemical hydrogen ***,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous ***,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution ***,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to *** remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion *** findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond.

关键词： Ammonia borane Hydrogen generation Hydrolysis Cobalt phosphide nanosheets Photocatalysis

Crystallinity-defect matching relationship of g-C_(3)N_(4): Experimental and theoretical perspectives

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Green Energy & Environment 2024年第4期9卷 623-658页

作者： Yuhan Li Ziteng Ren Zhengjiang He Ping Ouyang Youyu Duan Wendong Zhang Kangle Lv Fan Dong Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Key Laboratory of Catalysis and New Environmental MaterialsChongqing Technology and Business UniversityChongqing400067China Nanchang Institute of Technology Nanchang33044China key laboratory of Resources Conversion and Pollution Control of the state ethnic affairs commission College of Resources and Environmental ScienceSouth-Central Minzu UniversityWuhan430074China College of Physics and Center of Quantum Materials and Devices Chongqing UniversityChongqing401331China Chongqing key laboratory of Green Synthesis and Application Chongqing Normal UniversityChongqing401331China

Good crystallinity can reduce the charge recombination centers caused by defects,whilst structures with strong polycondensation have high charge mobility,leading to more charge transfer to the material surface for *** effort has been put into the preparation of a highly efficient g-C_(3)N_(4) with defects to improve its application potential under the premise in high ***,this review paper emphasizes the importance to balance the defect and crystallinity of g-C_(3)N_(4).In addition,detailed discussion on the relationship between defects and activity of g-C_(3)N_(4) was carried out based on its applications in environmental purification(e.g.,VOCs oxidation,NO_(x) oxidation,H_(2)O_(2) evolution,sterilization,pesticide oxidation)and energy conversion(H_(2) evolution,N_(2) fixation and CO_(2) reduction).Lastly,the challenge in developing more efficient defective g-C_(3)N_(4) photocatalytic materials is summarized.

关键词： Photocatalysis Defect G-C_(3)N_(4) Crystallinity Application

The chlorine evolution reaction promoted by organocatalysts with amide functional groups

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Science China chemistry 2024年第3期67卷 749-750页

作者： Lan Zhao Liang-Nian He state key laboratory and Institute of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

Since the nineteenth century, the chlor-alkali process entails the electrochemical oxidation of sodium chloride solutions to Cl_(2) by the chlorine evolution reaction(CER) and the simultaneous production of sodium hyd... 详细信息

关键词： chlorine hydroxide promoted