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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 key 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

Atomic Ni directional-substitution on ZnIn_(2)S_(4) nanosheet to achieve the equilibrium of elevated redox capacity and efficient carrier-kinetics performance in photocatalysis

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Journal of Energy chemistry 2024年第1期88卷 272-281,I0007页

作者： Haibin Huang Guiyang Yu Xingze Zhao Boce Cui Jinshi Yu Chenyang Zhao Heyuan Liu Xiyou Li School of Materials Science and Engineering China University of Petroleum(East China)Qingdao 266580ShandongChina key laboratory of optic-electric sensing and analytical chemistry for life Science(MOE) College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina College of New Energy China University of Petroleum(East China)Qingdao 266580ShandongChina

It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.

关键词： ZnIn_(2)S_(4) Substitution Carrier kinetics Redox capacity Photocatalysis

Surface/Interface Engineering of Hierarchical MoO_(2)/MoNi_(4)@Ru/RuO_(2)Heterogeneous Nanosheet Arrays for Alkaline Water Electrolysis with Fast Kinetics

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Chinese Journal of chemistry 2024年第2期42卷 119-128页

作者： Qiong Zhang Ruixue Zhang Yingxiu Zhao Tiantian Sun Jianyang Gao Guang-Rui Xu Zexing Wu Yu Yang Lei Wang key laboratory of Eco-chemical Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry of Life ScienceTaishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringSchool of Materials Science and EngineeringQingdao University of Science and TechnologyQingdaoShandong 266042China College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdaoShandong 266042China

Realizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production,while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half-cell reactions of water splitting.Here,we propose an approach of hydrothermal and thermal annealing methods for robust MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalyst with multiplying surface-active sites by depositing a monolayer amount of Ru.Benefiting from abundant MoO_(2)/MoNi_(4)@Ru/RuO_(2)heterointerfaces,MoO_(2)/MoNi_(4)@Ru/RuO_(2) heterogeneous cuboid array electrocatalysts effectively drive the alkaline water splitting with superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)performances.The synthesized MoO_(2)/MoNi_(4)@Ru/RuO_(2) has high HER activity,which realizes the working overpotentials of 48 mV at 50 mA·cm^(-2),further achieving overpotentials of 230 mv for industry-level 1000 mA·cm^(-2) in alkaline water electrolysis.Moreover,it also showed an enhanced OER activity than commercial RuO_(2) with a small overpotential of 280 mV at 200 mA·cm^(-2) in alkaline media.When building an electrolyzer with electrodes of(-)MoO_(2)/MoNi_(4)@Ru/RuO_(2)IIMo02/MoNig@Ru/RuO_(2)(+),a cell voltage of 1.63 V and 1.75 V is just required to support the current density of 200 mA·cm^(-2) and 500 mA-cm^(-2) in alkaline water electrolysis,much lower than that of the electrolyzer of(-)Pt/CIIRuO_(2)(+).This work demonstrates that MoO_(2)/MoNig@Ru/RuO_(2) heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications,providing a possibility for the exploration of water electrolysis with a large currentdensity.

关键词： Hierarchical heterostructure Surface engineering Bifunctional catalysts Hydrogen evolution reaction Oxygen evolution reaction Watersplitting Catalytic activity Electrocatalysis Heterogeneous catalysis

Stable multi-electron reaction stimulated by W doping VS_(4)for enhancing magnesium storage performance

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Journal of Energy chemistry 2024年第2期89卷 89-98,I0004页

作者： Yuxin Tian Jiankang Chen Guofeng Wang Bing Sun Alan Meng Lei Wang Guicun Li Jianfeng Huang Shiqi Ding Zhenjiang Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina key laboratory of optic-electric sensing and analytical chemistry for life Science MOEShandong Key Laboratory of Biochemical AnalysisCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021ShaanxiChina

Rechargeable magnesium batteries(RMBs)hold promise for offering higher volumetric energy density and safety features,attracting increasing research interest as the next post lithium-ion batteries.Developing high performance cathode material by inducing multi-electron reaction process as well as maintaining structural stability is the key to the development and application of RMBs.Herein,multielectron reaction occurred in VS_(4)by simple W doping strategy.W doping induces valence of partial V as V^(2+)and V^(3+)in VS_(4)structure,and then stimulates electrochemical reaction involving multi-electrons in 0.5%W-V-S.The flower-like microsphere morphology as well as rich S vacancies is also modulated by W doping to neutralize structure change in such multi-electron reaction process.The fabricated 0.5%W-V-S delivers higher specific capacity(149.3 m A h g^(-1)at 50 m A g^(-1),which is 1.6 times higher than that of VS_(4)),superior rate capability(76 mA h g^(-1)at 1000 mA g^(-1)),and stable cycling performance(1500cycles with capacity retention ratio of 93.8%).Besides that,pesudocapaticance-like contribution analysis as well as galvanostatic intermittent titration technique(GITT)further confirms the enhanced Mg^(2+)storage kinetics during such multi-electron involved electrochemical reaction process.Such discovery provides new insights into the designing of multi-electron reaction process in cathode as well as neutralizing structural change during such reaction for realizing superior electrochemical performance in energy storage devices.

关键词： Multi-electron reaction W doping Stable structure Cathode Rechargeable magnesium batteries

Fluoro-functionalized plant biomass adsorbent:Preparation and application in extraction of trace perfluorinated compounds from environmental water samples

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Journal of Environmental sciences 2024年第3期137卷 703-715页

作者： Xi Tan Yan Shi Chun-Feng Ma Quan Chi Yu-Hang Yang Wen-Xiang Zhang Hua-Ming Xiao Xian Wang key laboratory of analytical chemistry of the State Ethnic Affairs Commission School of Chemistry and Materials ScienceSouth-Central Minzu UniversityWuhan 430074China School of Pharmaceutical sciences South-Central Minzu UniversityWuhan 430074China key laboratory of Oilseeds Processing of Ministry of Agriculture Hubei Key Laboratory of Lipid Chemistry and NutritionOil Crops Research Institute of the Chinese Academy of Agricultural SciencesWuhan 430062China

Perfuorinated compounds(PFCs)are toxic and widely present in the environment,and therefore effective adsorbents are required to remove PFCs from environmental water.In the present study,a new type of fuorinated biomass materials was synthesized via an ingenious fuorosilanization reaction.These adsorbents were applied for the adsorption of 13typical PFCs,including perfuorocarboxylic acids(PFCAs)and perfuorosulfonic acids(PFSAs).By comparing their adsorption performance,Fluorinated cedar slag(FCS)was discovered to have the best absorption efficiency and enabled highly efficient enrichment of PFCs.The adsorption recovery of FCS with the investigated PFCs is greater than 90%under the optimal adsorption condition.Ascribed to the high affinity of F-F sorbent-sorbate interaction,FCS had good adsorption capacities of PFCs from aqueous solution,with the maximum adsorption capacity of 15.80 mg/g for PFOS and 10.71 mg/g for PFOA,respectively.Moreover,the adsorption time could be achieved in a short time(8 min).Using the FCS absorbent,an innovative FCS-solid phase extraction assisted with high performance liquid chromatography-electrospray-tandem mass spectrometry(FCS-SPE-HPLC-ESI-MS/MS)method was first developed to sensitively detect PFCs in the environmental water samples.The intra-day and inter-day recovery rates of the 13 compounds ranged from 90.7%-104.3%,with the RSD of 2.1%-4.7%(intra-day)and 2.5%-8.5%(inter-day),respectively.This research demonstrates the potential of the newly fuoro-functionalized plant biomass to adsorb PFCs from environmental water,with the advantages of high adsorption efficiencies,high antiinterference,easy operation and low economic cost.

关键词： Fluoro-functionalized biomass Perfuorinated compounds(PFCs) Adsorption efficiency Mass spectrometry(MS) Fluorinated cedar slag(FCS)

Advances of Electrochemical and Electrochemiluminescent Sensors Based on Covalent Organic Frameworks

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Nano-Micro Letters 2024年第2期16卷 395-422页

作者： Yue Cao Ru Wu Yan‑Yan Gao Yang Zhou Jun‑Jie Zhu key laboratory for Organic Electronics and Information Displays(KLOEID)and Institute of Advanced Materials(IAM) Nanjing University of Posts and Telecommunications(NJUPT)Nanjing 210023People’s Republic of China State key laboratory of analytical chemistry for life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023People’s Republic of China

Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.

关键词： Covalent organic frameworks Electrochemistry Electrochemiluminescence Sensors

Intracellular redox potential-driven live-cell synthesis of CdSe quantum dots in Staphylococcus aureus

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Science China chemistry 2024年第3期67卷 990-999页

作者： Cai-Qin Wu An-An Liu Xu Li Jia-Wei Tu Juan Kong Ling-Ling Yang Jian-Hong Jia Chuan Wang Bin Hu Zhi-Xiong Xie Dai-Wen Pang The Institute for Advanced Studies College of Chemistry and Molecular SciencesCollege of Life SciencesHubei Key Laboratory of Cell HomeostasisWuhan UniversityWuhan 430072China Research Center for analytical sciences College of ChemistryState Key Laboratory of Medicinal Chemical BiologyTianjin Key Laboratory of Biosensing and Molecular RecognitionFrontiers Science Center for New Organic MatterFrontiers Science Center for Cell Responsesand Haihe Laboratory of Sustainable Chemical TransformationsNankai UniversityTianjin 300071China

Biosynthesized semiconductor quantum dots(QDs) have bright fluorescence,adjustable particle sizes,and environmental friendliness,endowing them with convenience and potential for biological applications.Due to the unclear mechanism of the cellular environment on the live-cell synthesis of QDs,it is still difficult to regulate their optical properties.Here,the critical role of the intracellular redox environment in regulating the fluorescence properties of biosynthesized CdSe QDs in Staphylococcus aureus(S.aureus) has been elucidated.The glutathione peroxidase(GPx) activity directly affects the intracellular H_(2)O_(2) produced in the SeO_(3)^(2-) reduction,which further manipulates the glutathione redox cycle to determine the content of low-valence Seintermediates.As a result,the fluorescence intensity of the synthesized CdSe QDs increases by 60% in the GPx overexpressed cells.The cellular redox potential that is controlled by the GSH redox cycle provides the driving force for the reduction of SeO_(3)^(2-),facilitating the synthesis of CdSe QDs in S.aureus cells.The proposed mechanism of the cellular redox state provides a new perspective for regulating the synthesis of semiconductor nanomaterials in live cells.

关键词： redox H_(2)O_(2) peroxidase quantum dot Staphylococcus aureus

Tumor-targeted self-assembled micelles reducing PD-L1 expression combined with ICIs to enhance chemo-immunotherapy of TNBC

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Chinese Chemical Letters 2024年第2期35卷 305-310页

作者： Hongda Zhu Kai Ma Rui Ruan Chaobo Yang Aqin Yan Jing Li Qi Yu Hongmei Sun Mingxing Liu Hongmei Zheng Jing Gao Xiaofang Guan Zhu Dai Yao Sun Cooperative Innovation Center of Industrial Fermentation (Ministry of Education & Hubei Province) Key Laboratory of Fermentation Engineering (Ministry of Education)National “111” Center for Cellular Regulation and Molecular PharmaceuticsSchool of Food and Biological EngineeringHubei University of TechnologyWuhan 430068China Hubei Cancer Hospital Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430079China National key laboratory of Green Pesticide College of ChemistryCentral China Normal UniversityWuhan 430079China key laboratory of Medical optics Suzhou Institute of Biomedical Engineering and TechnologyChinese Academy of SciencesSuzhou 215163China key laboratory of optic-electric sensing and analytical chemistry for life Science Ministry of EducationQingdao University of Science and TechnologyQingdao 266000China

Immune checkpoint inhibitors(ICIs)therapy targeting programmed cell death ligand 1(PD-L1)and programmed death protein 1(PD-1)had exhibited significant clinical benefits for cancer treatment such as triple negative breast cancer(TNBC).However,the relatively low anti-tumor immune response rate and ICIs drug resistance highlight the necessity of developing ICIs combination therapy strategies to improve the anti-tumor effect of immunotherapy.Herein,the immunomodulator epigallocatechin gallate palmitate(PEGCG)and the immunoadjuvant metformin(MET)self-assembled into tumor-targeted micelles via hydrogen bond and electrostatic interaction,which encapsulated the therapeutic agents doxorubicin(DOX)-loaded PEGCG-MET micelles(PMD)and combined with ICIs(anti-PD-1 antibody)as therapeutic strategy to reduce the endogenous expression of PD-L1 and improve the tumor immunosuppressive microenvironment.The results presented that PMD integrated chemotherapy and immunotherapy to enhance antitumor efficacy in vitro and in vivo,compared with DOX or anti-PD-1 antibody for the therapy of TNBC.PMD micelles might be a potential candidate,which could remedy the shortcomings of antibody-based ICIs and provide synergistic effect to enhance the antitumor effects of ICIs in tumor therapy.

关键词： Immunotherapy Tumor-targeted Self-assembled micelles Metformin Reducing PD-L1 expression TNBC

Insight into the synergistic effect of defect and strong interface coupling on ZnIn_(2)S_(4)/CoIn_(2)S_(4)heterostructure for boosting photocatalytic H_(2) evolution

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Journal of Energy chemistry 2024年第5期92卷 151-161页

作者： Xuehua Wang Tianyu Shi Xianghu Wang Aili Song Guicun Li Lei Wang Jianfeng Huang Alan Meng Zhenjiang Li College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina key laboratory of optic-electric sensing and analytical chemistry for life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina Qingdao Huanghai University Qingdao 266000ShandongChina School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021ShaanxiChina

Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.

关键词： Defect-guided heteroepitaxial growth Heterointerface coupling Photocatalytic H_(2)evolution Mechanism HVs-ZIS/CIS

Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of Applied chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research Institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering laboratory State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2