This study systematically discusses the multidimensional regulatory mechanisms of defect engineering on the atomic arrangement, electronic structure evolution, adsorption and desorption behavior, active site reconstruction, and stability control of LDH-based catalytic interfaces. It provides theoretical support and directional guidance for improving the electrocatalytic efficiency of LDH-based catalysts through defect engineering.

Layered double hydroxides (LDHs)-based electrocatalysts, owing to their structural designability and interface responsiveness, have emerged as promising candidates for constructing efficient non-noble metal electrocatalysts. Through interfacial structural modulation, defect engineering facilitates the exposure and activation of catalytic sites, ultimately boosting the electrocatalytic performance of LDH systems. This review analyzes the principle of interface structure design in LDHs driven by defect engineering. Then, the multidimensional regulatory mechanisms of defect engineering on the atomic arrangement, electronic structure evolution, adsorption and desorption behaviors, active site reconstruction, and stability control in the catalytic interface of LDHs are systematically discussed. Finally, this paper summarizes the key challenges that remain to be addressed and provides theoretical support and direction guidance for the construction of defect engineering-driven interfacially regulated efficient electrocatalytic systems.