Host Modification of Layered Double Hydroxide Electrocatalyst to Boost the Thermodynamic and Kinetic Activity of Oxygen Evolution Reaction

Abstract Layered double hydroxides (LDHs) are regarded as an earth‐abundant and highly efficient electrocatalyst for oxygen evolution reaction (OER). In this work, a systematic strategy is demonstrated to simultaneously optimize the OER thermodynamic and kinetic activity via introducing a series of transition and main group metal atoms into the NiFe‐LDH host layers. Typically, V, Co, and Cr dopants largely promote the intrinsic activity of NiFe‐LDH through the effective electron transfer from Fe 3+ in NiFe‐LDH laminate to the doping metals, while the introduction of V, Ti, and Mn into NiFe‐LDH facilitates the kinetics of water oxidation due to the increased conductivity induced by dopants. Furthermore, the detailed experiments and density functional theory calculations illustrate that the presence of suitable heteroatoms (V) lowers the activation energy barrier for OER rate‐limiting step as well as promotes the electron transfers by effective electronic modification. This work provides an effective strategy to modulate the OER activity of LDHs and determine their performance trends for a more rational design of high‐performed OER electrocatalysts.