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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li department of chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University State Key Laboratory of Surface Physics and department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable ***,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as *** key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon *** mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion *** method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Pd@Ir-LOD multienzyme utilizing endogenous lactate consumption cooperates with photothermal for tumor therapy

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Nano research 2024年第1期17卷 270-281页

作者： Zichen Ye Yun Li Jingchao Li Xinyan Hu Jinyang Zheng Gongxin Zhang Sijin Xiang Tianbao Zhu Zhide Guo Xiaolan Chen State Key Laboratory for Physical chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials and Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Molecular Vaccinology and Molecular Diagnostics&center for Molecular Imaging and Translational Medicine School of Public Health Xiamen UniversityXiamen 361102China The High Educational Key Laboratory for Biomedical Engineering&Key Laboratory of Fire Retardant materials of Fujian Province Department of BiomaterialsCollege of MaterialsXiamen UniversityXiamen 361102China

Lactic acid(LA)plays a major role in the occurrence,development,and spread of *** by its high accumulation in tumor site,a novel lactate oxidase(LOD)conjugated two-dimensional Pd@Ir nanoplatform(Pd@Ir-LOD,PIL)was fabricated to combine cascade reaction with photothermal for tumor *** detail,the overexpressed LA in tumor microenvironment(TME)was a key factor to activate the PIL-based cascade reaction:(1)Plenty of H_(2)O_(2)could be generated from LA by the catalysis of LOD with O_(2);(2)potent·OH was produced from H_(2)O_(2)due to the peroxidase(POD)-like activity of PIL;(3)meantime,PIL’s catalase(CAT)-like activity could decompose part H_(2)O_(2)into O_(2)to achieve the purpose of LA cyclic ***,the reduced glutathione(GSH)scavenging capability of PIL might protect the produced reactive oxygen species(ROS)from being cleared to further improve the cascade therapeutic *** importantly,PIL had excellent photothermal conversion efficiency(37.35%)and manifested a surprising temperature rising effect in *** together,the decreasing LA concentration,accumulation of high-toxic ROS,the depletion of GSH together with the higher intra-tumoral temperature potently enhanced in vivo antitumor ***,a promising therapeutic tactic based on PIL integrating endogenous LA consumption,chemodynamic therapy(CDT),and photothermal therapy(PTT)has been put forward.

关键词： lactate oxidase chemodynamic therapy photothermal therapy cascade reaction tumor microenvironment

Efficient wide-bandgap perovskite solar cells with open-circuit voltage deficit below 0.4 V via hole-selective interface engineering

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Science China chemistry 2024年第6期67卷 2102-2110页

作者： Xiaoyu Ji Shuo Zhang Furong Yu Huidong Zhang Liqing Zhan Yue Hu Wei-Hong Zhu Yongzhen Wu Key Laboratory for Advanced materials and Joint International research Laboratory of Precision chemistry and Molecular Engineering Shanghai Key Laboratory of Functional Materials ChemistryFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China School of chemistry University of EdinburghKing’s BuildingsEdinburghEH93FJUK

Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low ***,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 ***,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and *** assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase *** energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 *** V_(OC)-deficit(<0.40 V)is the lowest value reported for *** work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.

关键词： cyanovinyl phosphonic acid energy level alignment hole-selective material open-circuit voltage wide-bandgap perovskite

A multifunctional electrolyte additive for zinc-ion capacitors with low temperature resistant and long lifespan

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Journal of Energy chemistry 2024年第7期94卷 477-485页

作者： Ming Sun Zekai Zhang Shuqing Fu Yifan Zhang Ruoyu Wang Hongchun Mu Cheng Lian Wenqiang Wang Gengchao Wang Shanghai Engineering research center of Hierarchical Nanomaterials Shanghai Key Laboratory of Advanced Polymeric MaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsFrontiers Science Center for Materiobiology and Dynamic Chemistryand School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Aqueous zinc-ion capacitors (ZICs) are considered as potential candidates for next generation electrochemical energy storage devices due to their high safety and low ***,the existing aqueous ZICs usually have the problems of zinc dendrite growth and unsatisfactory performance at low ***,an erythritol (Eryt) additive with inhibition of zinc dendrites and anti-freezing capability was introduced into the *** experimental characterization and theoretical calculation confirm that the Eryt adsorbed on the surface of zinc anodes regulates the deposition orientation of Zn^(2+) and inhibits the formation of *** also reconstructs the solvation structure in the electrolyte to reduce water activity,enabling the electrolyte to have a lower freezing point for operation at low *** the assistance of Eryt,the Zn||Zn symmetric cell exhibits a long cycle life of 2000 h,while the ZIC assembled with activated carbon (AC) cathode and zinc anode (Zn||AC) maintains a capacity retention of 98.2% after 30,000 cycles at a current density of 10 A g^(-1)(even after 10,000 cycles at-20°C,the capacity retention rate reached 94.8%.).This work provides a highly scalable,low-cost and effective strategy for the protection of the anodes of low-temperature aqueous ZICs.

关键词： Zinc-ioncapacitors Electrolyte additive Dendrite-free Freeze-resistant electrolyte

Removal of rubidium from brine by an integrated film of sulfonated polysulfone/graphene/potassium copper ferricyanide

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Chinese Journal of Chemical Engineering 2024年第5期69卷 112-121页

作者： Huanxi Xu Peihua Lin Pei-Jun Liu Hai-Gang Liu Hui-Bin Guo Chao-Xiang Wu Ming Fang Xu Zhang Guan-Ping Jin Anhui Province Engineering research center of Flexible and Intelligent materials School of Chemistry and Chemical EngineeringHefei University of TechnologyHefei 230009China Chemical Design and research Institute Co. LTD of Qinghai ProvinceQinghai Engineering and Technology Research Center of Fine ChemicalXining 810008China

A novel integrated film of sulfonated polysulfone/graphene/potassium copper ferricyanide(KCuFC/SPSG)was used for selectively extracting rubidium ion(Rb^(+))from *** form KCuFC/SPSG,the precursor film of sulfonated polysulfone/graphene(SPSG)was synthesized by phase conversion process,which was alternately immersed in 0.1 mol·L^(-1)CuSO_(4)/K_(4)[Fe(CN)_(6)]by in-situ adsorption coupled co-precipitation *** data such as nuclear magnetic resonance spectrometer,Fourier transform infrared spectroscope,X-ray photoelectron spectroscope,X-ray diffraction,scanning electron microscope,and energy dispersive spectroscopy all verified that abundant KCuFC were uniformly located on the *** resulting KCuFC/SPSG was used in film separation *** the solution was fed into the system,the Rb^(+)could be selectively adsorption by KCuFC/*** the saturation adsorption,0.5 mol·L^(-1)NH_(4)Cl/HCl was fed into the film cell,Rb^(+)could be quickly desorbed by ion-exchange between Rb^(+)and NH_(4)^(+)in the lattice of *** purpose of separating and recovering Rb^(+)from the brine can be achieved after the repeated *** effects of pH,adsorption time,and interferential ions on the adsorption capacity of Rb^(+)were investigated by batch *** adsorption behavior fits the pseudo-second order kinetic process,while KCuFC has a higher adsorption capacity(Langmuir maximum sorption 165.4 mg·g^(-1)).In addition,KCuFC/SPSG shows excellent selectivity for Rb^(+)even in complex brine ***/SPSG could maintain 93.5%extraction efficiency after five adsorption/desorption cycles.

关键词： Rubidium extraction Potassium copper ferricyanide Sulfonated polysulfone Graphene oxide Adsorption

Synthesis of hierarchically porous carbon materials by zinc salts-assisted carbonization of biomass and organic solid wastes

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Particuology 2024年第1期84卷 45-52页

作者： Le-Le Zhang Lei Tong Yanwei Ding Wanqun Zhang Hai-Wei Liang Hefei National research center for Physical Sciences at the Microscale Department of ChemistryUniversity of Science and Technology of ChinaHefei230026China

Hierarchically porous carbons(HPCs)with multimodal pores have attracted considerable attention due to their unique physical and chemical properties and various application potentials in heterogeneous catalysis,environmental treatment,and energy storage and ***,we report a general and simple zinc salts-assisted method for the synthesis of HPCs with varied porosity and chemical func-tionalities by the direct carbonization of diverse biomass and *** the carbonization,zinc salts are thermally decomposed into nanoparticles that serve as in-situ templates to introduce nanopores in *** prepared HPCs exhibit high specific surface areas(up to 2432 m2 g-1),large pore volumes(up to 4.30 cm^(3)g^(-1)),and broad pore size ***,the zinc salts can be recovered and recycled,supporting the sustainable production of HPCs on large *** prepared HPCs-supported catalysts with atomically dispersed metal sites exhibit promising electrocatalytic performance for the oxygen reduction reaction.

关键词： Hierarchical porous carbon Zinc salts Biomass Wastes Electrocatalysis

Nb_(2)O_(5) nanocrystals decorated graphene composites as anode materials for high-performance dual-ion batteries

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Nano research 2024年第3期17卷 1535-1541页

作者： Lei Wang Fei Huang Guoyin Zhu Zhihui Dai Jiangsu Collaborative Innovation center of Biomedical Functional materials Jiangsu Key Laboratory of Biofunctional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China Institute of Advanced materials and Flexible Electronics(IAMFE) School of Chemistry and Materials ScienceNanjing University of Information Science&TechnologyNanjing 210044China School of chemistry and Molecular Engineering Nanjing Tech UniversityNanjing 211816China

Niobium oxide(Nb_(2)O_(5))is a promising material in photocatalytic,solar cell,electronic like electron field emitters,and especially lithium-ion batteries(LIBs)because of its adjustable morphologies,controllable crystal type,stable structure,and environmental ***,its low electrical conductivity lowers the rate performance and limits the practical applications in ***,we present a one-step solid-state synthesis of orthogonal Nb_(2)O_(5) nanocrystals/graphene composites(Nb_(2)O_(5)/G)as high-performance anode materials in *** from the nanoscale crystalline structure Nb_(2)O_(5) and highly-conductive graphene substrate,the as-prepared Nb_(2)O_(5)/G exhibits excellent electrochemical ***,a reversible structural phase transition between orthogonal Nb_(2)O_(5) and tetragonal Li1-xNbO_(2)(0

关键词： niobium oxide graphene anode dual-ion batteries graphite intercalation

General synthesis of transition metal nitride arrays by ultrafast flash Joule heating within 500 ms

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Science China chemistry 2024年第6期67卷 1976-1982页

作者： Peiqi Shen Jiahui Zhao Yanan Gao Yunxiang Lin Yuchen Han Kun Xu School of chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui ProvinceAnhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized MaterialsKey Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei230601China Institutes of Physical Science and Information Technology Center of Free Electron Laser&High Magnetic FieldLeibniz International Joint Research Center of Materials Sciences of Anhui ProvinceAnhui UniversityHefei230601China

Transition metal nitrides(TMNs)are considered as viable alternatives to noble metal catalysts owing to their versatile electronic structure and favorable catalytic ***,the conventional synthetic processes for TMNs suffer from high energy consumption and low production *** this study,a range of TMNs and their hetero-composite arrays were successfully synthesized via an ultrafast flash Joule heating technology within 0.5 *** a proof concept,the nitrides and hetero-composites were applied for the electrocatalytic hydrazine oxidation reaction(HzOR),in which the Co_(4)N/Mo_(16)N_(7)arrays shows the best performance with a geometric current density of 100 mA cm^(-2)at 23 mV(*** hydrogen electrode(RHE)).This work paves a new way for the ultrafast synthesis of TMNs which could meet the ever-increased energy crisis.

关键词： flash Joule heating rapid synthesis transition metal nitrides hydrazine oxidation reaction electrocatalysts

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Molecule configurations modulate packing array and charge transfer in cocrystal engineering

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Science China chemistry 2024年第2期67卷 512-516页

作者： Shenglong An Mengyuan Qiao Xin Jin Xuanying Chen Jianhua Su Lifang Guo Zhiyun Zhang Key Laboratory for Advanced materials and Joint International research Laboratory of Precision chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CentreFrontiers Science Center for Materiobiology and Dynamic ChemistryEast China University of Science&TechnologyShanghai200237China

Organic cocrystal as an emerging assembly strategy has received increasing attention in constructing multiple functional materials,through continually screening suitable constituent monomers or changing their stoichiometry ***,the role of molecule configuration in the cocrystal field is rarely explored despite the fascinating potential in regulating the packing *** this study,the N,N′-diphenyl-5,10-dihydrophenazine derivatives(DPPs) with the flexible scaffold and different methyl substitutions are selected as the donors bearing various molecular *** a simple collaborative way,a series of cocrystals based on DPPs and OFN(octafluoronaphthalene) are fabricated,exhibiting two self-adaptive molecular stacking arrays.X-ray crystallographic analysis and theoretical calculation unveil their different π···π interactions and charge transfer characters,leading to the significant emission redshift up to 125 nm compared with individual *** a result,controllable molecule stacking structure,tunable emission,and charge transfer properties can be *** study provides a new perspective to reveal the structure-property relationships at the molecular level by controlling the molecule configuration in cocrystal engineering,contributing to the development of cocrystal theoretical physics and organic functional materials.

关键词： cocrystals molecular configuration self-adaptive packing mode charge transfer