Evolution of catalyst structures and reaction intermediates during electroreduction CO2 toward C2+ product on Cu-based catalyst: An experimental and theoretical review

Carbon dioxide electroreduction reaction (CO2RR) to multicarbon (C2+) product catalyzed by Cu-based catalysts has been regarded as a reliable and efficient method to reduce air pollution and develop green energy. Apart from intermediate evolution, the structures of Cu-based catalysts go through a reconstruction during the electrolysis processes. However, pinpointing the reconstruction motivation, the structural reconstruction and reaction mechanism under operating conditions is challenging. The in situ/operando technologies and ab initio molecular dynamics calculation improve the possibility of addressing the challenge. In the article, recent utilizations of multiple in situ/operando characterization methods and ab initio molecular dynamics calculations in tracking structural reconstruction, discovering active sites, and unveiling reaction mechanisms are reviewed. Finally, based on the comprehensive studies, we concluded some problems for catalyst reconstruction and reaction mechanisms during CO2RR.