Atomic Coordination Regulation in Electronic Structure of Electrocatalysts

Abstract The electronic structure of electrocatalysts is central to energy conversion processes, determining catalytic efficiency, intrinsic activity, and stability. Precise regulation of atomic‐level coordination environments optimizes this electronic structure. This review analyzes the interplay between electrocatalyst electronic structure and coordination configuration through energy‐level matching theory and the Sabatier principle. Leveraging advanced characterization techniques, diverse bonding motifs—including unsaturated bonds, surface self‐bonds, interfacial chemical bonds, and 2D bonds are examined—and elucidate their mechanisms for modulating electronic properties. These insights demonstrate how coordination chemistry control via electronic structure engineering enables rational design of high‐performance electrocatalysts. Integration of advanced catalyst architectures exploiting quantum confinement with machine‐learning‐guided design, alongside characterization tools dynamically linking electronic states to performance, will accelerate next‐generation electrocatalyst development.