Structural Reconstruction of Catalysts in Electroreduction Reaction: Identifying, Understanding, and Manipulating.

Electroreduction transformation of small molecules (CO 2 , N 2 , and H 2 O) into chemical feedstocks offers a promising approach to eliminate carbon emissions and harness renewable energy. Most cathodic catalysts often undergo structural transformation under operating electroreduction conditions. These structural reconstructions are reflected in changes in their catalytic activity. In-depth understanding of the change of active sites and influence parameters of reconstruction behaviors is an essential precondition for the design of highly efficient catalysts. Despite the previous achievements, comprehensive insight toward the structural evolution mechanism in cathodic catalysts, compared to anode ones, under reaction conditions is still lacking. Herein, an overview of structural reconstruction for cathodic catalysts in terms of fundamental mechanisms, reconstruction process, advanced characterizations, and influencing parameters is provided. On this basis, the typical strategies for manipulating the structural reconfiguration of catalysts are also explicitly discussed from the catalyst structure and working environment. By delivering the mechanism, strategies, insights, and techniques, this review will provide a comprehensive understanding of the structural reconstruction of cathodic catalysts in electroreduction reactions and future guidelines for their rational development.