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

• Published in: Journal of energy chemistry Vol. 70; pp. 414 - 436
• Main Authors: Zhang, Wenbiao, Yang, Yang, Tang, Yi, Gao, Qingsheng
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.07.2022
• Subjects: CO2 reduction reaction; Electronic configurations; Hydrogen evolution reaction; In-situ reconstruction; Nitrogen reduction reaction; Topological changes; Valence states; Electronic configurations; Valence states; Nitrogen reduction reaction; Hydrogen evolution reaction; CO2 reduction reaction; In-situ reconstruction; Topological changes
• ISSN: 2095-4956
• DOI: 10.1016/j.jechem.2022.02.036

This review summarizes in-situ electrocatalyst reconstruction in electrocatalytic H2 evolution, and CO2 and N2 reduction, focusing on the correlations between reconfigured surface and performance. [Display omitted] Cathodic electrocatalytic reactions, such as hydrogen evolution and CO2/N2 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 H2 evolution and CO2/N2 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.