Dual-phase engineered hierarchical CoP enables dynamic reconstruction and multimetallic synergy for superior oxygen evolution

Cobalt phosphide (CoP) suffers from sluggish surface reconstruction kinetics and intrinsically low activity of reconstructed active sites during electrocatalytic processes. To address these limitations, a dual-phase engineering strategy is developed for synthesizing a hierarchical Mo, Fe co-doped CoP heterostructure encapsulated within boron and nitrogen co-doped carbon matrices (Mo, Fe-CoP/BNC). This architecture establishes a multimetallic regulation system synergized with conductive B, N-codoped carbon frameworks, enabling dynamic reconstruction and electronic structure optimization. In 1.0 M KOH electrolyte, the optimized catalyst exhibits superior oxygen evolution performance with a low overpotential of 272 mV at 10 mA·cm −2 and exceptional durability exceeding 120 h of continuous operation. Combined experimental characterization and density functional theory (DFT) calculations reveal the structural origins of enhanced performance: Partial leaching of high-valent Mo 6+ induces in-situ surface reconstruction of CoP into highly active CoOOH species, significantly increasing accessible active sites; Fe dopants enable reversible Fe 2+ /Fe 3+ redox cycling, providing dynamic electron transfer pathways while modulating the d -band center of Co sites to optimize intermediate adsorption energetics; Boron co-doping synergistically tailors local charge distribution and coordination environments, facilitating homogeneous elemental dispersion and structural stability. This study not only develops a high-performance oxygen evolution reaction (OER) electrocatalyst but also elucidates the intrinsic mechanism of structure reconstruction-electronic modulation synergy in enhancing catalytic activity through combined experimental and theoretical investigations.