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in-situ reconstruction of catalysts in cathodic electrocatalysis: New insights into active-site structures and working mechanisms

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Journal of Energy Chemistry 2022年第7期31卷 414-436,I0011页

作者： Wenbiao Zhang Yang Yang Yi Tang Qingsheng Gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632GuangdongChina Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials(iCHEM)Fudan UniversityShanghai 200433China

Cathodic electrocatalytic reactions, such as hydrogen evolution and CO_(2)/N_(2) reduction, are the key processes that store intermittent electricity into stable chemical energy. Although a great progress has been made to boost activity and selectivity via elaborative catalyst design, the structure–property relationships have not been sufficiently understood in the context of surface reconfiguration under working conditions. Recent efforts devoted to tracking dynamic evolution of electrocatalysts using in-situ and/or operando techniques gave new insights into the real structure and working mechanism of active sites,and provided principles to design better catalysts. The achievement of cathodic electrocatalysts in this subject is herein summarized, focusing on the correlations between reconstructed surface and electrocatalytic performance. Briefly, the thermodynamics of reconstruction at cathodes is discussed at first, and then the representative progresses in H_(2) evolution and CO_(2)/N_(2) reduction are introduced in sequence to acquire insights into electrochemical processes on in-situ reconfigured surfaces or interfaces. Finally, a perspective is offered to guide future investigations. This review is anticipated to shed some new light on in-depth understanding cathodic electrocatalysis and exploiting prominent electrocatalysts.

关键词： Hydrogen evolution reaction CO_(2)reduction reaction Nitrogen reduction reaction in-situ reconstruction Electronic configurations Valence states Topological changes

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