“…As a star material, the controllable pore size, large specific surface area, dispersed active sites, and diverse topology of metal–organic frameworks (MOF) composed of organic ligands and metal nodes, especially Ni, Fe, Co, etc., endow MOF with outstanding electrocatalytic properties. , However, the poor electrical conductivity and low availability of active sites have been the existing problems of MOF as electrocatalytic materials. , To address these shortcomings for efficient overall water splitting, the crystal structure of MOF acts as a key factor in measuring the electrocatalytic performance. The modulation of the crystal structure and coordination environment of metal–organic frameworks is a straightforward and essential way to reduce the energy barrier and impedance of the electrocatalyst reaction. , Generally, there are three ways to regulate the intrinsic electronic structure of MOF based on both metal clusters and ligands: (1) doping the second and third metals to partially replace the initial metal sites; (2) introducing missing linkers to compete with the original organic ligand; (3) the addition of a regulator to introduce defects.…”