Enriched electrophilic oxygen species facilitate acidic oxygen evolution on Ru-Mo binary oxide catalysts  

作　　者：Yaya Wang Yunzhou Wen Yumeng Cheng Xinhong Chen Mengjiao Zhuansun Tongbao Wang Jun Li Debora Meira Huarui Sun Jun Wei Jia Zhou Yuhang Wang Sisi He 

机构地区：[1]Shenzhen Key Laboratory of Flexible Printed Electronics Technology,Harbin Institute of Technology(Shenzhen),University Town,Shenzhen 518055,China [2]School of Science,Harbin Institute of Technology(Shenzhen),University Town,Shenzhen 518055,China [3]Institute of Functional Nano&Soft Materials(FUNSOM),Jiangsu Key Laboratory of Advanced Negative Carbon Technologies,Soochow University,Suzhou 215123,China [4]Frontiers Science Center for Transformative Molecules,Shanghai Jiao Tong University,Shanghai 200240,China [5]Science Division,Canadian Light Source,Saskatoon,SK,S7N 2V3,Canada [6]Photon Science Division,Argonne National Laboratory,Lemont,IL,60439,USA [7]School of Materials Science and Engineering,Harbin Institute of Technology,(Shenzhen),University Town,Shenzhen 518055,China

出　　处：《Nano Research》2024年第3期1165-1172,共8页纳米研究（英文版）

基　　金：support from the National Natural Science Foundation of China(No.52103300);the Guangdong Basic and Applied Basic Research Foundation(No.2023A1515010572);the Shenzhen Science and Technology Program(Nos.JCYJ20210324132806017 and GXWD20220811163904001);the Innovation Material Research Center of Harbin Institute of Technology,Shenzhen for the instrumentation assistance.Y.H.W.acknowledges the funding support from the National Natural Science Foundation of China(No.22179088);the Natural Science Foundation of Jiangsu Province of China(No.BK20210699);the National Natural Science Fund for Excellent Young Scientists Fund Program(Overseas);the Program for Jiangsu Specially-Appointed Professors,the Program of Soochow Innovation and Entrepreneurship Leading Talents(No.ZXL2022450);the start-up supports of Soochow University,Suzhou Key Laboratory of Functional Nano&Soft Materials,the Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 Project,the Joint International Research Laboratory of Carbon-Based Functional Materials and Devices.J.Z.acknowledges the funding support from the State Key Laboratory of Urban Water Resources&Environment(Harbin Institute of Technology)(No.2022TS36);Computer time made available by the National Supercomputing Center of China in Shenzhen(Shenzhen Cloud Computing Center)is gratefully acknowledged.J.L.acknowledges the start-up funding support from Shanghai Jiao Tong University(No.WH220432516);This research used synchrotron resources of the Advanced Photon Source,an Office of Science User Facility operated for the US Department of Energy Office of Science by Argonne National Laboratory and was supported by the US Department of Energy under contract No.DE-AC02-06CH11357 and the Canadian Light Source and its funding partners.

摘　　要：The polymer electrolyte membrane(PEM)electrolyzers are burdened with costly iridium(Ir)-based catalysts and high operation overpotentials for the oxygen evolution reaction(OER).The development of earth-abundant,highly active,and durable electrocatalysts to replace Ir is a critical step in reducing the cost of green hydrogen production.Here we develop a Ru5Mo4Ox binary oxide catalyst that exhibits high activity and stability in acidic OER.The electron-withdrawing property of Mo enriches the electrophilic surface oxygen species,which promotes acidic OER to proceed via the adsorbate evolution pathway.As a result,we achieve a 189 mV overpotential at 10 mA·cm^(-2) and a Tafel slope of 48.8 mV·dec^(-1).Our catalyst demonstrates a substantial 18-fold increase in intrinsic activity,as evaluated by turnover frequency,compared to commercially available RuO_(2) and IrO_(2) catalysts.Moreover,we report a stable OER operation at 10 mA·cm^(-2) for 100 h with a low degradation rate of 2.05 mV·h^(-1).

关 键 词：ELECTROCATALYSIS oxygen evolution reaction(OER) ruthenium(Ru)-based oxide molybdenum electrophilic oxygen 

分 类 号：O64[理学—物理化学]