MoCx/CoP Janus Structure Embedded Carbon Frame for Boosting Hydrazine Oxidation and Hydrogen Evolution Reactions

Abstract The integration of hydrazine electrooxidation (HzOR) and hydrogen evolution reaction (HER) presents an efficient pathway for high‐purity hydrogen production. However, developing bifunctional catalysts remains challenging for the demands of multiple active‐centers and tailored electronic properties. Here, a unique Janus nano‐catalysts of MoC x /CoP embedded on carbon frameworks (MoC x /CoP@C) is introduced, featuring dual electronic states (depletion and accumulation)driven by charge redistribution within MoC x /CoP, acting as dual active‐sites (DAS) for both HER and HzOR. Theoretical analysis reveals these independent DAS in MoC x /CoP significantly enhance catalytic activity for both HER and HzOR. Specifically, accumulated electrons at MoC x /CoP interfaces weaken the bonding strength of N‐H in N 2 H 4 , thereby decreasing dehydrogenation energy barrier while electronic‐deficient Mo sites within MoC x accelerate H * desorption, thus promoting HER kinetics. This catalyst exhibits ultra‐low potential of −73 mV at 10 mA cm −2 for anodic HzOR, comparable to noble catalysts and low overpotential of 95 mV at 10 mA cm −2 for cathodic HER. When employed in an overall hydrazine splitting (OHzS) system, MoC x /CoP@C shows promising commercial potential, with low energy consumption (0.16 V), high Faradaic efficiency (95.4%) and long‐term stability. This study underscores the feasibility of designing independent DAS catalysts and elucidates the mechanistic origins of bifunctional activities.