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Particuology 2024年第6期89卷 99-108页

作者： Weihao Liu Huanhuan He Qingtao Liu Xin Wan Jianglan Shui School of Materials Science and Engineering Beihang UniversityBeijing100191China School of Space and Environment Beihang UniversityBeijing102206China Tianmushan Laboratory Hangzhou310023China

The excellent oxygen reduction reaction(ORR)activity of fe–n–c catalysts in acidic media makes them potential for low-cost proton exchange membrane fuel cells.In recent years,it has been shown that heteroatoms(B,O,S,P,cl,F,etc.)can be used as electron-withdrawing groups to modulate the planar structure and electron distribution of the fe–nx active sites to achieve simultaneous improvement of catalytic activity and stability.However,the optimal location of the heteroatoms remains unclear.Here,taking chalcogen heteroatoms(S and Se)as an example,we control the doping positions and investigate their effect on the ORR performance of the fe–n–c catalysts.The first coordination shell of the iron single atom is identified as the optimal doping position.The optimized catalysts fe–n_(3)Se_(1)/nc and fe–n_(3)Se_(1)/nc demonstrate improved activity and stability in both half cells and fuel cells.This work provides insights into the enhancement mechanism of heteroatom doping in single-atom catalysts.

关键词： Oxygen reduction reaction fe-n-c catalysts Hetero-atom doping Doping position Enhancement mechanism

Secondary-Atom-Doping Enables Robust fe-n-c Single-Atom catalysts with Enhanced Oxygen Reduction Reaction

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nano-Micro Letters 2020年第11期12卷 281-291页

作者： Xin Luo Xiaoqian Wei Hengjia Wang Wenling Gu Takuma Kaneko Yusuke Yoshida Xiao Zhao chengzhou Zhu Key Laboratory of Pesticide and chemical Biology of Ministry of Education International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079People’s Republic of China Innovation Research center for Fuel cells The University of Electro-CommunicationsChofugaokaChofuTokyo 182‑8585Japan

Single-atom catalysts(SAcs) with nitrogen-coordinated nonprecious metal sites have exhibited inimitable advantages in electrocatalysis.However,a large room for improving their activity and durability remains.Herein,we construct atomically dispersed fe sites in n-doped carbon supports by secondary-atom-doped strategy.Upon the secondary doping,the density and coordination environment of active sites can be efficiently tuned,enabling the simultaneous improvement in the number and reactivity of the active site.Besides,structure optimizations in terms of the enlarged surface area and improved hydrophilicity can be achieved simultaneously.Due to the beneficial microstructure and abundant highly active fen_5 moieties resulting from the secondary doping,the resultant catalyst exhibits an admirable half-wave potential of 0.81 V versus 0.83 V for Pt/c and much better stability than Pt/c in acidic media.This work would offer a general strategy for the design and preparation of highly active SAcs for electrochemical energy devices.

关键词： Single-atom catalysts fe-n-c catalysts Doping Porous nanostructures Oxygen reduction reaction

fe-n-c catalysts for PEMFc: Progress towards the commercial application under DOE reference

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Journal of Energy chemistry 2019年第12期28卷 77-87页

作者： Lina Wang Xin Wan Shuangyu Liu Li Xu Jianglan Shui School of Materials Science and Engineering Beihang UniversityBeijing 100083China Material Laboratory of State Grid corporation of china Global Energy Interconnection Research InstituteBeijing 102211China

Proton exchange membrane fuel cells(PEMFc)have attracted much attention because of their high energy conversion efficiency,high power density and zero emission of pollutants.However,the high cost of the cathode platinum group metal(PGM)catalysts creates a barrier for the large-scale application of PEMFc.Tremendous efforts have been devoted to the development of low-cost PGM-free catalysts,especially the fe-n-c catalysts,to replace the expensive PGM catalysts.However,the characterization methods and evaluation standards of the catalysts varies,which is not conducive to the comparison of PGM-free catalysts.U.S.Department of energy(DOE)is the only authority that specifies the testing standards and activity targets for PGM-free catalysts.In this review,the major breakthroughs of fe-n-c catalysts are outlined with the reference of DOE standards and targets.The preparation and characteristics of these highly active fe-n-c catalysts are briefly introduced.Moreover,the efforts on improving the mass transfer and the durability issue of fe-n-c fuel cell are discussed.Finally,the prospective directions concerning the comprehensive evaluation of the fe-n-c catalysts are proposed.

关键词： PEMFc fe-n-c catalysts U.S.DOE Test standards Activity targets

Engineering fe‑n_(4)Electronic Structure with Adjacent co‑n_(2)c_(2)and co nanoclusters on carbon nanotubes for Efficient Oxygen Electrocatalysis

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纳微快报:英文版 2023年第12期15卷 283-297页

作者： Mingjie Wu Xiaohua Yang Xun cui ning chen Lei Du Mohamed cherif Fu‑Kuo chiang Yuren Wen Amir Hassanpour Francois Vidal Sasha Omanovic Yingkui Yang Shuhui Sun Gaixia Zhang State Key Laboratory of new Textile Materials and Advanced Processing Technologies Wuhan Textile UniversityWuhan 430200People’s Republic of China Institut national de la Recherche Scientifique(InRS) Center Energie Materiaux TelecommunicationsVarennesQC J3X 1P7Canada Department of chemical Engineering McGill University3610 University StreetMontrealQC H3A 0C5Canada Department of Electrical Engineering Ecole de Technologie Superieure(ETS)MontrealQC H3C 1K3Canada canadian Light Source(cLS) 44 Innovation BoulevardSaskatoonSK S7N 2V3Canada national Institute of Low-carbon-and-clean-Energy Beijing 102211People’s Republic of China School of Materials Science and Engineering University of Science and Technology BeijingBeijing 100083People’s Republic of China

Regulating the local configuration of atomically dispersed transition-metal atom catalysts is the key to oxygen electrocatalysis performance enhancement.Unlike the previously reported singleatom or dual-atom configurations,we designed a new type of binary-atom catalyst,through engineering fe-n_(4)electronic structure with adjacent co-n_(2)c_(2)and nitrogen-coordinated co nanoclusters,as oxygen electrocatalysts.The resultant optimized electronic structure of the fe-n_(4)active center favors the binding capability of intermediates and enhances oxygen reduction reaction(ORR)activity in both alkaline and acid conditions.In addition,anchoring M-n-c atomic sites on highly graphitized carbon supports guarantees of efficient charge-and mass-transports,and escorts the high bifunctional catalytic activity of the entire catalyst.Further,through the combination of electrochemical studies and in-situ X-ray absorption spectroscopy analyses,the ORR degradation mechanisms under highly oxidative conditions during oxygen evolution reaction processes were revealed.This work developed a new binary-atom catalyst and systematically investigates the effect of highly oxidative environments on ORR electrochemical behavior.It demonstrates the strategy for facilitating oxygen electrocatalytic activity and stability of the atomically dispersed M-n-c catalysts.

关键词： Atomically dispersed fe-n-c catalysts ORR/OER Rechargeable zinc-air battery Fuel cells

fe-n-c电催化氧还原反应催化剂的研究进展

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Science china Materials 2022年第7期65卷 1701-1722页

作者：王颖王蕾付宏刚 Key Laboratory of Superlight Materials and Surface Technology of Ministry of Education College of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001China Key Laboratory of Functional Inorganic Material chemistry Ministry of Education of ChinaHeilongjiang UniversityHarbin 150080China

氧还原反应(ORR)是燃料电池和金属-空气电池等各种能源转换器件中重要的半反应.由于ORR的动力学缓慢,需要开发高活性电催化剂来替代常用的贵金属铂基催化剂.fe-n-c催化剂被认为是最有前景的材料,其丰富的活性位点可以降低含氧中间体的能... 详细信息

氧还原反应(ORR)是燃料电池和金属-空气电池等各种能源转换器件中重要的半反应.由于ORR的动力学缓慢,需要开发高活性电催化剂来替代常用的贵金属铂基催化剂.fe-n-c催化剂被认为是最有前景的材料,其丰富的活性位点可以降低含氧中间体的能垒.在这篇综述中,我们详细总结了fe-n-c催化剂在理论和实验研究方面的最新研究进展.首先,概述了基于fe-n-c催化剂的电催化ORR的反应机理.然后,对fe-n-c催化剂的设计策略和活性位点进行了分类.接下来,讨论了活性位点与催化性能之间的关系.介绍了fe-n-c催化剂在燃料电池和锌空气电池中的应用现状.最后,进一步提出了fe-n-c催化剂在可控合成、机理研究和能源器件应用方面面临的挑战和机遇.

关键词： fe-n-c catalysts oxygen reaction mechanisms physical characterizations design strategies theoretical calculations fuel cells Zn-air battery