Confinement Engineering of Zinc Single‐Atom Triggered Charge Redistribution on Ruthenium Site for Alkaline Hydrogen Production

Abstract Optimizing the interaction between metal and support in the supported metal catalysts effectively refines the electronic structure and boosts the catalytic properties of loaded active components. Herein a method is introduced to confine ultrafine ruthenium (Ru) nanoparticles within atomically dispersed Zn‐N₄ sites on a N‐doped carbon network (Ru/Zn‐N‐C) through the strong electronic metal–support interaction, achieving superior catalytic activity and stability for alkaline hydrogen evolution. Spectroscopic data and theoretical modeling elucidate that the remarkable catalytic performance of Ru sites stems from their strong electronic coupling with neighboring Zn‐N₄ moiety and pyridinic N/pyrrolic N. This interaction induces an electron‐deficient state of Ru, thereby accelerating the dissociation of H₂O and lowering the energy barriers for the desorption of OH* and H*. This insight provides a deeper understanding of the catalytic mechanisms at play. Furthermore, alkaline water electrolyzer using this catalyst as cathode delivers a mass activity of 3 A mg_cat^–1 at 2.0 V, much surpassing Ru‐C. This research opens a novel pathway for the development of advanced materials , tailored for energy storage and conversion applications.