The critical role of electrochemically activated adsorbates in neutral OER

作     者：Longsheng Zhang Haiyang Yuan Liping Wang Hui Zhang Yijing Zang Yao Tian Yunzhou Wen Fenglou Ni Hao Song Haifeng Wang Bo Zhang Huisheng Peng 张龙生;袁海洋;王丽平;章辉;臧易静;田瑶;温蕴周;倪凤楼;宋浩;王海丰;张波;彭慧胜

作者机构：State Key Laboratory of Molecular Engineering of PolymersDepartment of Macromolecular Science and Laboratory of Advanced MaterialsFudan UniversityShanghai 200438China Key Laboratory for Advanced MaterialsKey Laboratory for Advanced MaterialsCentre for Computational Chemistry and Research Institute of Industrial CatalysisEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Functional Materials for InformaticsShanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesCAS Center for Excellence in Superconducting ElectronicsShanghai 200050China Key Laboratory of Systems BioengineeringSchool of Chemical Engineering and TechnologySynBio Research PlatformCollaborative Innovation Centre of Chemical Science and EngineeringTianjin UniversityTianjin 300072China 

出 版 物：《Science China Materials》 (中国科学（材料科学（英文版）)

年 卷 期：2020年第63卷第12期

页      面：2509-2516页

核心收录：

学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the Ministry of Science and Technology(2016YFA0203302) the National Natural Science Foundation of China(21875042,21634003,51573027 and 11227902) Science and Technology Commission of Shanghai Municipality(16JC1400702 and 18QA1400800) Shanghai Municipal Education Commission(2017-01-07-00-07-E00062) Yanchang Petroleum Group the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning 

主　　题：electrocatalysis oxygen evolution reaction adsorbates neutral electrolytes 

摘      要：Developing efficient electrocatalysts for the oxygen evolution reaction(OER)under neutral conditions is important for microbial electrolysis cells(MECs).However,the OER kinetics in neutral electrolytes at present are extremely sluggish,resulting in high overpotentials that greatly limit the energy conversion efficiencies of *** studies failed to probe the adsorbates on surface metal sites of catalysts at the atomic scale and elucidate their influence on the catalytic activities,which has impeded the rational design of efficient neutral OER catalysts with optimal surface ***,using in situ transmission electron microscopy(TEM),in situ X-ray photoelectron spectroscopy(XPS)and in situ low-energy ion scattering studies,we have identified,for the first time,that the electrochemically activated adsorbates on surface metal sites play a critical role in boosting the neutral OER activities of Ru-Ir binary oxide(RuxIryO2)*** adsorbate-activated RuxIryO2on a glassy carbon electrode achieved a low overpotential of 324 m V at10 m A cm-2in neutral electrolyte,with a 36-fold improvement in turnover frequency compared with that of Ir *** application in an MEC system,the resulting full cell showed a decreased voltage of 1.8 V,200 m V lower than the best value reported to date,facilitating efficient synthesis of poly(3-hydroxybutyrate)from bioelectrochemical *** functional theory(DFT)studies revealed that the enhanced OER activity of RuxIryO2catalyst arose from local structural distortion of adjacent adsorbate-covered Ru octahedra at the catalyst surface and the consequently decreased adsorption energies of OER intermediates on Ir active center.