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Special Issue of Single-atom Catalysis

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Chemical Research in Chinese Universities 2022年第5期38卷 I0001-I0004页

作者： wu yuen SU Chenliang WANG Yanggang University of Science and Technology of China Hefei 230026P.R.China Shenzhen University Shenzhen 518060P.R.China Southern University of Science and Technology Shenzhen 518055P.R.China

Single-atom catalysts(SACs)are a new type of heterogeneous catalysts formed by isolated metal atoms anchored on kinds of substrates.SACs are distinctly distinguished from traditional catalysts by characterizing with unique electronic structure,quantum size effect and unsaturated coordination environment,etc.,which brought subverted effects on traditional catalytic fields once upon the emergence.The unique chemical and physical properties impart SACs with outstanding catalytic performance,embodying nearly 1o0%atom utilization,high catalytic activity and excellent durability.SACs invariably have been the"hotspot"in catalysis research field during the last decade,shining brilliantly in applications of electro-,photo-and thermal catalysis.In particular,the advent of SACs points towards a possibility of the substantial cost reduction of precious metal catalysts in the future.This themed issue selected advanced studies on design,synthesis,characterization,and application of SACs,dedicating to assisting readers in a comprehensively and in-depth understanding of SACs.

关键词： durability catalysis invar

A Supported Palladium on Gallium-based Liquid Metal Catalyst for Enhanced Oxygen Reduction Reaction

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Chemical Research in Chinese Universities 2022年第5期38卷 1219-1225页

作者： MA Chunrong SONG Bingyi MA Zhentao WANG Xiaoqian TIAN Lin ZHANG Haoran CHEN Cai ZHENG Xusheng YANG Li-ming wu yuen First Affiliated Hospital of USTC Division of Life Sciences and MedicineUniversity of Science and Technology of ChinaHefei 230026P.R.China Dalian National Laboratory for Clean Energy Dalian 116023P.R.China Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica Key Laboratory of Material Chemistry for Energy Conversion and StorageMinistry of EducationHubei Key Laboratory of Materials Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074P.R.China National Synchrotron Radiation Laboratory(NSRL) University of Science and Technology of ChinaHefei 230029P.R.China

Developing high-performance catalysts for oxygen reduction reaction to replace costly platinum-based materials is of great importance but still confronted with challenges.Herein,a kind of supported palladium liquid metal catalyst,which is prepared by galvanic replacement,surpasses commercial Pt/C and Pd/C in oxygen reduction catalysis with a higher half-wave potential of 0.92 V,mass activity of 1.85 A/mgPd at 0.90 V,and superior durability.The liquid metal support can both optimize the electronic structures of Pd sites and guarantee the dispersion of Pd atoms,which explains the enhanced activity and durability,respectively.This work opens an avenue for rational design of catalysts.

关键词： Liquid metal Supported catalyst Oxygen reduction Electrocatalysis

Single-atom Catalysts for Polymer Electrolyte Membrane Fuel Cells

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Chemical Research in Chinese Universities 2020年第3期36卷 320-328页

作者： ZHU Mengzhao WANG Jing wu yuen Department of Chemistry iChEM(Collaborative Innovation Center of Chemistryfor Energy Materials)University of Science and Technology of ChinaHefei 230026P.R.China

Searching for high-activity,stabilily and highly casbellective electrocalalysts for acid oxygen reaction rolutioo(ORR)has always been a urgent problem in polymer ectrolyte menbrane fuel ells(PEMFC).Nonetheless,the electrochemical poperties of various systems have their intrinsic limits and tremendous eforts have been paid oul to search for highly eficient electocatalysts by more raional control over the size,morphology,compoition,and structure.In particular,single-atom catalysts(SACs)have atrascted extensive intenest due to theirs cxcellant activity,stability,slctivity and the highest metal tiliztion In rceat yeurs,the number of papers in the field of SACs has incressed rapidly,indicating that SACs have made great progress.This review foouses on SACs electo-echemical applications in the acid ORR and introduces immovative syntheses,fiuel cell performance and long-time durabilily.

关键词： Singe-aton catalyst Oxygen reactio reduction Polymer electrolyte membrane fuel cell

Acid-stable antimonate based catalysts for the electrocatalytic oxygen evolution reaction

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Nano Research 2023年第4期16卷 4691-4697页

作者： Xiaoping Gao Huang Zhou Zhe Wang Gang Zhou Jin Wang yuen wu College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China Preservation Technology Advanced Research CenterHefei Hualing Co.LtdHefei 230000China School of Science Hubei University of TechnologyWuhan 430068China

Acid-stable and highly active catalysts for the electrocatalytic oxygen evolution reaction(OER)are paramount to the advancement of electrochemical technologies for clean energy conversion and utilization.In this work,based on the density functional theory(DFT)calculations,we systematically investigated the MSb_(2)O_(6)(M=Fe,Co,and Ni)and transition metal(TM)doped MSb_(2)O_(6)(TM-MSb_(2)O_(6),TM=Mn,Fe,Co,Ni,Cu,Zn,Ru,Rh,Pd,Ir,and Pt)as potential antimonate-based electrocatalysts for the OER.The stability and OER activity of these considered electrocatalysts were systematically studied under acidic conditions.It was found that Rh-NiSb_(2)O_(6),Pt-CoSb_(2)O_(6),Rh-FeSbO4,and Co-NiSb_(2)O_(6)can serve as efficient and stable OER electrocatalysts,and their OER catalytic activities are better than that of the current state-of-the-art OER catalyst(IrO2).Our findings highlight a family of promising antimonate-based OER electrocatalysts for future experimental verification.

关键词： oxygen evolution reaction antimonates acid-stable oxides electrocatalysis density functional theory

Total conversion of centimeter-scale nickel foam into single atom electrocatalysts with highly selective CO_(2)electrocatalytic reduction in neutral electrolyte

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Nano Research 2023年第2期16卷 2003-2010页

作者： Qikui Fan Pengfei Gao Shan Ren Yunteng Qu Chuncai Kong Jian Yang yuen wu Ministry of Education Key Laboratory for Non-equilibrium Synthesis and Modulation of Condensed Matter Shaanxi Province Key Laboratory of Advanced Functional Materials and Mesoscopic PhysicsSchool of PhysicsXi’an Jiaotong UniversityXi’an 710049China Shenzhen Key Laboratory of Special Functional Materials Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Northwest Institute of Nuclear Technology Xi’an 710024China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China State Key Laboratory of Photoelectric Technology and Functional Materials International Collaborative Center on Photoelectric Technology and Nano Functional MaterialsInstitute of Photonics and Photon-TechnologyNorthwest UniversityXi’an 710069China Department of Chemistry iChEM(Collaborative Innovation Center of Chemistry for Energy Materials)University of Science and Technology of ChinaHefei 230026China

To improve the atomic utilization of metals and reduce the cost of industrialization,the one-step total monoatomization of macroscopic bulk metals,as opposed to nanoscale metals,is effective.In this study,we used a thermal diffusion method to directly convert commercial centimeter-scale Ni foam to porous Ni single-atom-loaded carbon nanotubes(CNTs).As expected,owing to the coating of single-atom on porous,highly conductive CNT carriers,Ni single-atom electrocatalysts(Ni-SACs)exhibit extremely high activity and selectivity in CO_(2)electroreduction(CO_(2)RR),yielding a current density of>350 mA/cm^(2),a selectivity for CO of>91%under a flow cell configuration using a 1 M potassium chloride(KCl)electrolyte.Based on the superior activity of the Ni-SACs electrocatalyst,an integrated gas-phase electrochemical zero-gap reactor was introduced to generate a significant amount of CO current for potential practical applications.The overall current can be increased to 800 mA,while maintaining CO Faradaic efficiencies(FEs)at above 90%per unit cell.Our findings and insights on the active site transformation mechanism for macroscopic bulk Ni foam conversion into single atoms can inform the design of highly active single-atom catalysts used in industrial CO_(2)RR systems.

关键词： Ni single atom electrocatalyst CO_(2)electroreduction to CO neutral electrolyte thermal diffusion

Surface modification of MoS_(2) nanosheets by single Ni atom for ultrasensitive dopamine detection

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Nano Research 2023年第1期16卷 917-924页

作者： Xuejiao Sun Cai Chen Can Xiong Congmin Zhang Xusheng Zheng Jin Wang Xiaoping Gao Zhen-Qiang Yu yuen wu College of Chemistry and Environmental Engineering Institute of Low-dimensional Materials Genome InitiativeShenzhen UniversityShenzhen 518071China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071China Dalian National Laboratory for Clean Energy Dalian 116023China National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029China

Single atom catalysts have been recognized as potential catalysts to fabricate electrochemical biosensors,due to their unexpected catalytic selectivity and activity.Here,we designed and fabricated an ultrasensitive dopamine(DA)sensor based on the flower-like MoS_(2) embellished with single Ni site catalyst(Ni-MoS_(2)).The limit of detection could achieve 1 pM in phosphate buffer solution(PBS,pH=7.4),1 pM in bovine serum(pH=7.4),and 100 pM in artificial urine(pH=6.8).The excellent sensing performance was attributed to the Ni single atom axial anchoring on the Mo atom in the MoS_(2) basal plane with the Ni-S_(3) structure.Both the experiment and density functional theory(DFT)results certify that this structural feature is more favorable for the adsorption and electron transfer of DA on Ni atoms.The high proportion of Ni active sites on MoS_(2) basal plane effectively enhanced the intrinsic electronic conductivity and electrochemical activity toward DA.The successful establishment of this sensor gives a new guide to expand the field of single atom catalyst in the application of biosensors.

关键词： single atom catalysts MoS_(2) dopamine(DA)sensor serum urine

Cu_(2+1)O/CuO_(x)heterostructures promote the electrosynthesis of C^(2+)products from CO_(2)

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Nano Research 2023年第4期16卷 4698-4705页

作者： Rongbo Sun Cong Wei Zixiang Huang Shuwen Niu Xiao Han Cai Chen Haoran Wang Jia Song Jun-Dong Yi Geng wu Dewei Rao Xusheng Zheng yuen wu Gongming Wang Xun Hong Center of Advanced Nanocatalysis(CAN) Department of Applied ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China National Synchrotron Radiation Laboratory(NSRL) University of Science and Technology of ChinaHefei 230026China

Manipulating the oxidation state of Cu catalysts can significantly affect the selectivity and activity of electrocatalytic carbon dioxide reduction(CO_(2)RR).However,the thermodynamically favorable cathodic reduction to metallic states typically leads to catalytic deactivation.Herein,a defect construction strategy is employed to prepare crystalline/amorphous Cu_(2+1)O/CuO_(x)heterostructures(c/a-CuO_(x))with abundant Cu0 and Cuδ+(0<δ<1)sites for CO_(2)RR.The C^(2+)Faradaic efficiency of the heterostructured Cu catalyst is up to 81.3%,with partial current densities of 406.7 mA·cm−2.Significantly,real-time monitoring of the Cu oxidation state evolution by in-situ Raman spectroscopy confirms the stability of Cuδ+species under long-term high current density operation.Density functional theory(DFT)calculations further reveal that the adjacent Cu0 and Cuδ+sites in heterostructured c/a-CuO_(x)can efficiently reduce the energy barrier of CO coupling for C^(2+)products.

关键词： CO_(2)electroreduction C-C coupling heterostructures in-situ Raman manipulation of oxidation states

Surface Br?nsted-Lewis dual acid sites for high-efficiency dinitrogen photofixation in pure water

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Journal of Energy Chemistry 2022年第4期67卷 824-830页

作者： Cai Chen Jiewei Chen Zhiyuan Wang Fei Huang Jian Yang Yunteng Qu Kuang Liang Xiao Ge Yanggang Wang Hui Zhang yuen wu College of Chemistry and Chemical Engineering Southwest Petroleum University Department of Chemistry Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and Technology School of Chemistry and Materials Science iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Shenyang National Laboratory for Materials Science Institute of Metal Research Chinese Academy of Sciences

As is known to all, nitrogen not only plays an important role in the industrial development of human society but also plays an important part in the proteins that constitute the essence of life[1]. In 1910, the Haber-... 详细信息

关键词： Photocatalytic nitrogen fixation Brønsted-Lewis dual acid sites Surface-modified TiO2 Surface states F and H atoms

Formic acid oxidation by iridium single-atom catalysts on nitrogendoped carbon

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Science China Chemistry 2020年第9期63卷 1171-1172页

作者： Huang Zhou yuen wu Hefei National Laboratory for Physical Sciences at the Microscale Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China

The challenge of the depletion of traditional fossil fuels forces researchers to develop sustainable and highly effective energy storage and conversion technologies.Direct formic acid fuel cells(DFAFCs)exhibit great potential applications in small,lightweight and long-lasting portable power sources,due to the inherent advantages of formic acid,e.g.,safer and easier to store and handle than hydrogen,faster electro-oxidation kinetics than ethanol and lower fuel crossover through the Nafion membrane than methanol[1].

关键词： kinetics methanol faster