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Synthesis of Axially Coordinated Cobalt Porphyrin/graphene Oxide Nanocomposite for Enhanced Electrocatalytic CO_(2) Reduction to CO

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Chinese Journal of Structural Chemistry 2022年第3期41卷 1-11,I0007页

作者： YOU Wei-Feng XU Xiao CAO Ai-Hui TAO Zhi-Jie KANG Long-Tian Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China

The electrocatalysts containing cobalt-pyrrolic nitrogen-carbon(Co-N_(4)-C)moiety for CO_(2)reduction reaction(CO_(2)RR)have caught much ***;the effects of Co valence state and its synergy with gra-phene substrate are not clear *** this work;cobalt porphyrin(CoTPP)molecule with the intrinsic Co-N_(4)-C moiety is successfully combined with graphene oxide(GO)via three kinds of liquid-phase *** ratio of CoTPP to GO and the valence state of Co atom are studied to explore their catalysis for CO_(2)RR to *** is found that axial-ly-coordinated Co(III)TPPCl/GO nanocomposites synthesized via a chemical method exhibit better ability for CO_(2)RR;as compared with Co(II)TPP+GO and/or Co(III)TPPCl+GO nanocomposites obtained via a physically mixing *** optimizing the ratio of CoTPP to GO;the Faradaic efficiency(FE)is more than 90%for CO_(2)RR to CO between−0.7 and−0.8 V *** hydrogen electrode(RHE)in Co(III)TPPCl/*** synergy be-tween CoTPP and GO and the effect of Co valence state are systematically investigated;indicating that their strong interaction plays the key role in electrocatalytic CO_(2)RR.

关键词： cobalt porphyrin graphene oxide axial coordination carbon dioxide reduction synergistic catalysis

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The Enhancement of Selectivity and Activity for Two-Electron Oxygen Reduction Reaction by Tuned Oxygen Defects on Amorphous Hydroxide Catalysts

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CCS Chemistry 2022年第2期4卷 566-583页

作者： Junheng Huang Changle Fu Junxiang Chen Nangan Senthilkumar Xinxin Peng Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of the Chinese Academy of Science Beijing 100049

Amorphous catalysts,thanks to their uniquely coordinated unsaturated properties and abundance of defect sites,tend to possess higher activity and selectivity than their crystalline *** this work,we report a facile and general solventcontrolled precipitation method to prepare hybrids of graphene oxide(GO)supporting amorphous metal hydroxide[A-M(OH)_(x)/GO,M=Cu,Co,and Mn],which provides us with tangible materials to study the structure–performance relationship of various amorphous *** systematic investigation of A-Cu(OH)_(2)/GO by coupling ex situ/in situ characteristic techniques with electrochemical studies reveals that electrocatalytic activity and selectivity toward a two-electron oxygen reduction reaction(ORR)is highly dependent on the coordinated Cu catalytic sites and the disordered structure of A-Cu(OH)_(2).In situ X-ray absorption near-edge structure(XANES)and density functional theory(DFT)calculation verify that the degree of OH*poisoning(ΔG0 OH*)tuned by three-OH-coordinated Cu sites in amorphous structures plays a crucial role in selective catalysis of ORR for H_(2)O_(2) *** optimized A-Cu(OH)_(2)/GO shows superior activity and high selectivity(~95%)toward H_(2)O_(2),as demonstrated by a zinc–air battery capable of on-site H_(2)O_(2) production with a rate as high as 3401.5 mmol h^(−1) g^(−1).

关键词： amorphous hydroxide general preparation two-electron ORR on-site H_(2)O_(2)production three-OH-coordinated Cu sites

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Unraveling the reaction mechanism of high reversible capacity CuP_(2)/C anode with native oxidation PO_(x) component for sodium-ion batteries

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Chinese Chemical Letters 2025年第1期36卷 574-578页

作者： Huixin Chen Chen Zhao Hongjun Yue Guiming Zhong Xiang Han Liang Yin Ding Chen State Key Laboratory of Advanced Design and Manufacturing for Vehicle Body College of Mechanical and Vehicle EngineeringHunan UniversityChangsha 410082China CAS key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Materials Science and Engineering Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesNanjing Forestry UniversityNanjing 210037China Laboratory of Advanced Spectro-electrochemistry and Li-ion Batteries Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Institute of Physics Chinese Academy of SciencesBeijing 100190China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi institutesChinese Academy of SciencesXiamen 361021China

Phosphorus-based anode is a promising anode for sodium-ion batteries(SIBs)due to its high specific capacity,however,suffers from poor electronic conductivity and unfavorable electrochemical *** metals such as copper(Cu)into phosphorus has been demonstrated to not only improve the electronic conductivity but also accommodate the volume change during cycling,yet the underline sodiation mechanism is not ***,take a copper phosphide and reduced graphene oxide(CuP_(2)/C)composite as an example,which delivers a high reversible capacity of>900 mAh/***,it is revealed that the native oxidation PO_(x)components of the CuP_(2)/C composite show higher electrochemical reversibility than the bulk Cu P_(2),based on a quantitative analysis of high-resolution solid-state^(31)P NMR,ex-situ XPS and synchrotron X-ray diffraction characterization *** sodiation products Na_(3)PO_(4) and Na_(4)P_(2)O_(7) derived from PO_(x) could react with Na-P alloys and regenerate to PO_(x) during charge process,which probably accounts for the high reversible capacity of the Cu P_(2)/C *** findings also illustrate that the phosphorus transforms into nanocrystalline Na_(3)P and Na_(x)P alloys,which laterally shows crystallization-amorphization evolution process during cycling.

关键词： CuP_(2)/C composite POx component Reaction mechanism Solid-state NMR Sodium-ion batteries

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Constructing a high concentration CuO/CeO_(2) interface for complete oxidation of toluene:The fantastic application of spatial confinement strategy

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Journal of Rare Earths 2023年第6期41卷 850-861,I0002页

作者： Chao Wang Yan Li Huiao Liu Ziying Hu Xinhui Hao Hongpeng Jia Jing Chen Canzhong Lu CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China Xiamen Institute of Rare-earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China Institute of Urban Environment Chinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China

In this paper,CeO_(2) substrate was prepared by the sol-gel method,further CuO was introduced by adding the copper complexes with chelating agents into the sol-gel precursors of CeO_(2),in which different chelating agents(β-cyclodextrin,glucose and trimesic acid)were *** synthesis method helps the CuO species to disperse very uniformly in the CeO_(2) *** the amount of copper oxide is up to33 mol%,the CuO/CeO_(2) samples can still maintain a highly dispersed *** CeO_(2) and CuO/CeO_(2)samples were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),temperature-programmed reduction of hydrogen(H_(2)-TPR),temperature-programed desorption(O_(2)-TPD),*** is found that the CuO/CeO_(2) catalyst prepared byβ-cyclodextrin(βCuO/CeO_(2)) exhibits better catalytic performance owing to the higher dispersion,higher specific surface area,more defects,more active Ce3+and Cu^(+) ions,more oxygen vacancies,more surface active oxygen,relatively better low temperature reducibility,and the exposed(110) active *** the condition of 1000×10-6toluene in air and WHSV=60000 mL/(g·h),the T90for toluene conversion is 227℃.The reaction mechanism of toluene catalytic oxidation over CeO_(2)andβCuO/CeO_(2) is discussed by the study of in-situ *** work affords a simple and efficient method for the synthesis of highly dispersed bimetal oxide catalysts with high contents.

关键词： Catalytic oxidation Toluene Confinement strategy Chelating agent Rare earths Copper

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Dynamic atomic observations in electrochemical interfaces

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National Science Review 2024年第9期11卷 110-111页

作者： Hao Zhang Yu Zhang Zhenhai Wen Department of Chemical Engineering Massachusetts Institute of Technology Department of Chemistry University of Oxford CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Materials and Techniques toward Hydrogen Energy Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences

Direct detection of the solid-liquid electrochemical interface(ESLI) dynamics at the atomic scale is crucial for understanding and optimizing electrochemical reactions [1], yet traditional imaging techniques struggle with capturing these details due to the masking effects of liquid environments and the complexity of dynamic processes [2]. In recent years, researchers have been able to achieve realtime observation and analysis of ESLI structural changes and behaviors during electrochemical reactions at high resolution,

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Selective recovery of Th(Ⅳ) from radioactive rare earth waste residue by utilizing MoS_(2)-modified ion-absorbed type rare earth tailings

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Journal of Rare Earths 2024年第9期42卷 1782-1791,I0005页

作者： Xirong Chen Xinyu Fu Yun Gao Zhiyuan Zeng Bin Huang Xiaoqi Sun Faculty of Materials Metallurgy and Chemistry Jiangxi University of Science and TechnologyGanzhou341000China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Fujian Research Center for Rare Earth Engineering Technology Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China Fujian College University of Chinese Academy of SciencesFuzhou350002China Jiangxi Province Key Laboratory of Cleaner Production of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhouJiangxi341000China

In the process of extracting ion-absorbed rare earth ore(IREO),the production of radioactive waste is a major environmental *** address this issue,MoS_(2) was used to modify ion-absorbed rare earth tailings(RET) to synthesize a novel MoS_(2)@RET composite material for the effective handling of radioactive waste generated in IREO separation *** composite material was thoroughly characterized using various analytical techniques,including X-ray diffraction(XRD),X-ray photoelectron spectroscopy(XPS),thermogravimetry(TG),Fourier-transform infrared(FTIR),scanning electron microscopy(SEM),Brunaue r-Emmett-Teller(BET) and energy dispersive spectroscopy(EDS).By optimizing the operating parameters,the optimal experimental conditions were determined to be pH=3,contact time=60 min,liquid-solid ratio=6 g/L,and initial concentration=150 mg/*** adsorption data fitted well with the pseudo second-order rate *** thermodynamic parameters concerning the adsorption of Th(Ⅳ) were analyzed and *** isotherm model is a more fitting choice for the adsorption process compared to the Freundlich isotherm ***_(2)@RET was used in the acid leachate of IREO waste residue,achieving the separation of Th and rare earth *** mechanism of Th(Ⅳ) adsorption by MoS_(2)@RET was investigated,revealing that the adsorption process involves electrostatic interactions,chemical bonding,and redox *** above research results indicate that MoS_(2)@RET composite materials have application potential in the sustainable treatment of IREO radioactive waste.

关键词： Rare earths Thorium Radioactive waste residue Adsorption Separation

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Lanthanide-Doped Inorganic Nanoprobes for Luminescent Assays of Biomarkers

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Accounts of Materials Research 2023年第2期4卷 193-204页

作者： Luping Wang Siyuan Han Chenliang Li Datao Tu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials and State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108 China University of Chinese Academy of Sciences Beijing 100049 China

Tremendous progress in nanomaterial and nanotechnology has been made in recent years,which greatly contributes to the development of inorganic nanoparticles(NPs)as luminescent probes in diverse biomedical *** particular,these luminescent nanoprobes are widely employed for sensitive assays of biomarkers like disease ***,the luminescent bioassay technologies mainly rely on conventional molecular probes such as lanthanide(Ln3+)chelates or organic dyes,which suffer from inferior photochemical stability,low photobleaching,potential long-term toxicity,or high background *** contrast,Ln3+-doped NPs possess distinct physicochemical properties including better photostability,lower toxicity,and superior optical properties like long photoluminescent(PL)lifetime,narrow emission band,and tunable spectral range from the ultraviolet to the second near-infrared(NIR-II),which make them extremely ideal as luminescent *** such,enormous research enthusiasm has been invested in this fascinating field of Ln3+-doped luminescent nanoprobes in recent ***,background-free luminescent bioassays with high signal-to-noise have been achieved by employing Ln3+-doped NPs on the basis of their downshifting luminescence(DSL)with a long PL lifetime,NIR-II luminescence with long-wavelength emissions,or upconverting luminescence(UCL)upon NIR ***,there are still key challenges for Ln3+-doped nanoprobes owing to their low brightness and quantum yield,which restrict their biomedical *** the past decade,we have explored efficient approaches for the synthesis and design of highly efficient Ln3+-doped nanoprobes toward ultrasensitive luminescent bioassay of disease *** this Account,we summarize our most recent endeavors toward the development of inorganic Ln3+-doped NPs as sensitive nanoprobes for luminescent ***,we overview the approaches of controlled synthesis and optical manipulation to obtain highly e

关键词： properties luminescence lifetime

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Pre-fixing defects in carbon framework for revealing the active sites of oxygen reduction reaction at nitrogen-doped carbon nanotubes

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Journal of Energy Chemistry 2021年第12期30卷 521-527,I0012页

作者： Bing Huang Kun Hou Yang Liu Rongtao Hu Lunhui Guan CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 FujianChina University of Chinese Academy of Sciences Beijing 100049China

Nitrogen-doped carbon-based materials are promising non-platinum group metal electrocatalysts for the oxygen reduction reaction(ORR).Understanding their ORR active sites is vital for the rational design and development of nitrogen-doped carbon-based electrocatalysts with enhanced catalytic efficiency and ***,the conclusive analysis of the ORR mechanism of nitrogen-doped carbon-based electrocatalysts remains a grand challenge because the catalysts have a complex inhomogeneous ***,we elucidate this problem using nitrogen-doped carbon nanotubes framework catalysts with fixed defect concentrations prepared by pre-thermal treatment at a low *** generation of defects under high-temperature treatment was effectively suppressed to enable a simple model for ORR mechanism study.A correlation between ORR pathways and the different nitrogen species in the nitrogen-doped carbon catalysts was revealed through a combination of structural and electrochemical properties ***,our results also demonstrate the importance of defects for *** believe that the results will provide instructive guidance for designing and developing novel carbon nanomaterials for ORR.

关键词： Electrocatalysts Oxygen reduction reaction Defects Nitrogen-doped carbon nanotube

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A high-tortuosity holey graphene in-situ derived from cytomembrane/cytoderm boosts ultrastable potassium storage

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Journal of Materials Science & Technology 2023年第8期139卷 69-78页

作者： Jun Xiao Xin Min Yue Lin Qiyao Yu Wei Wang Xiaowen Wu Yangai Liu Zhaohui Huang Minghao Fang Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes National Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of Geosciences(Beijing)Beijing100083China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Sciences Beijing100049China State Key Laboratory of Explosion Science and Technology School of Mechatronical EngineeringBeijing Institute of TechnologyBeijing100081China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing100083China

The sluggish K^(+)kinetics and structural instability of the generally-used graphite and other carbon-based materials hinder the development of potassium-ion batteries(PIBs)for high-rate capability and long-term ***,inspired by the unique flake structure and chemical composition of cytomembrane and cytoderm,we design high-tortuosity holey graphene as a highly efficient anode for *** flake cytomembrane and cytoderm shrink into wrinkled morphology during drying and sintering and then convert into high-tortuosity graphene after oxidative exfoliating and thermal reducing ***-while,the proteins,sugars,and glycolipids embedded in cytomembrane and cytoderm can in-situ form nanoholes with highly abundant oxygenic groups and heteroatoms around,which can be easily removed and finally the high-tortuosity holey graphene is obtained after a thermal reducing *** stress distribution after K^(+)intercalation confirms the optimized release of strain caused by the volume change through the finite element *** from the unique nanoholes shortening the ion-diffusion length,the synergy of wrinkled and holey structure stabilizing volume fluctuation,and the enhanced electronic conductivity and specific surface area,the high-tortuosity holey graphene demonstrates high reversible capacities of 410 mAh g^(-1)at 25 mA g^(-1)after 150 cycles and retains 91.5%at 2 A g^(-1)after 2500 cycles.

关键词： Potassium-ion batteries Graphene High tortuosity Cytomembrane and cytoderm Anode

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CeO_(2)quantum-dots engineering 3D carbon architectures toward dendrite-free Na anode and reversible Te cathode for high-performance Na-Te batteries

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InfoMat 2022年第10期4卷 90-101页

作者： Yangjie Liu Junwei Li Xiang Hu Jun Yuan Guobao Zhong Lu Zhang Junxiang Chen Hongbing Zhan Zhenhai Wen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujianChina College of Materials Science and Engineering Fuzhou UniversityFuzhouChina Department of Chemical Engineering KU LeuvenHeverleeBelgium

Sodium-tellurium(Na-Te)battery,thanks to high theoretical capacity and abundant sodium source,has been envisaged as one promising battery technology,its practical application yet faces daunting challenges regarding how to mitigate the critical issues of uncontrollable dendrites growth at Na anode and polytellurides shuttling effect at Te *** here report an elaborative design for fabrication of microsphere skeleton nanohybrids with three-dimensional(3D)hierarchical porous carbon loading CeO_(2)quantum dots(CeO_(2)-QDs/HPC),which feature highly favorable properties of sodiophilic and catalysis for hosting sodium and tellurium,*** systematic investigations coupling with first-principle calculations demonstrate the CeO_(2)-QDs/HPC not only offers favorable structure and abundant electrocatalytic sites for facilitating interconversion between Te and NaxTe as a cathode host,but also can function as dendrite inhibitor anode host for reversible sodium electro-plating/*** Na-Te battery exhibits admiring electrochemical performance with an impressive specific capacity of 392 mAh g1,a long cycling stability over 1000 cycles,as well as remarkably high energy density of 192 Wh kg1 based on the total mass of anode and *** proof-of-concept bifunctional host design for active electrode materials can render a new insight and direction to the development of high-performance Na-Te batteries.

关键词： CeO_(2)quantum dots dual-functional hosts hierarchical porous carbon microsphere skeleton nanohybrids Na-Te batteries

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