Advances in Understanding the Electrocatalytic Reconstruction Chemistry of Coordination Compounds

Abstract Coordination compounds including mainstream metal‐organic frameworks and Prussian blue analogues receive extensive researches when they directly serve as electrocatalysts. Their reconstruction phenomena, that are closely associated with actual contributions and intrinsic catalytic mechanisms, are expected to be well summarized. Here, the recent advances in understanding reconstruction chemistry of coordination compounds are reviewed, including their main classifications and structural properties, reconstruction phenomena in electrocatalysis (e.g., oxygen/hydrogen evolution reaction, CO₂ reduction), influence factors of reconstruction parameters (e.g., reconstruction rate and reconstruction degree), and reconstruction‐performance correlation. It is outlined that the reconstruction processes are influenced by electronic structure of coordination compounds, pH and temperature of testing solution, and applied potentials. The characterization techniques reflecting the evolution information before and after catalysis are also introduced for reconstruction‐related mechanistic study. Finally, some challenges and outlooks on reconstruction investigations of coordination compounds are proposed, and the necessity of studying and understanding of these themes under actual working conditions of devices is highlighted.