Strongly Coupled NiMo@Alloy‐LDH Interfaces with Low‐Barrier Schottky Junctions for Oxygen Evolution Reaction

Abstract The main challenge in developing Schottky‐contact OER catalytic devices based on layered double hydroxides (LDHs) is to achieve metal–semiconductor junctions with low contact resistance and high charge transfer capacity. However, due to the presence of high potential barriers and Fermi pinning, conventional Schottky contacts are usually unsatisfactory, resulting in poor‐working electrode performance and high energy consumption. In this study, a new concept of “hindrance factor” is introduced to quantify the difficulty of electron transfer, and a low‐hindrance factor Schottky contact formed by strong coupling of semiconductor LDH and NiMo alloy clusters is designed. This interface guides charge redistribution, optimizes the bonding and orbital states of adsorption sites, and enhances the targeted adsorption of OH intermediates. The results show that the configured NiMo@NiFeCe‐LDH working electrode only needs 1.445 V (vs RHE) to drive the reaction and shows excellent durability in 400 h of testing. At the same time, based on this study, a strategy for screening high‐performance Schottky junctions is developed. This strategy provides a bridge for studying interface properties, orbital hybridization, and charge transfer, reveals the potential mechanism for reducing contact resistance, and has important guiding significance for screening high‐performance metal–semiconductor electrocatalysts and stability.