Delicate Control Over Electron Distribution and Water Dissociation Kinetics in Strongly Coupled Ru@NMoC Hybrid Catalyst Realizes Efficient Seawater Electrolysis

Abstract Delicate control over electron distribution in hybrid catalysts is crucial for improving hydrogen evolution catalysis, which remains an aspirational target in advancing efficient hydrogen production. Herein, we optimize the local electronic structures and balance the reaction steps by incorporating Ru clusters into nitrogen‐doped molybdenum carbide (denoted as Ru@NMoC), addressing performance limitations in alkaline seawater. The Ru@NMoC catalyst demonstrates ultralow overpotentials of 8, 17, and 20 mV at 10 mA cm⁻ 2 in 1 M KOH, 1 M KOH + 0.5 M NaCl, and 1 M KOH seawater, respectively, significantly outperforming conventional HER catalysts. Operando spectroscopic techniques reveal strong ability for interface water dissociation and stable local charge structure in Ru@NMoC. Theoretical simulations demonstrate that N‐doping of Ru clusters self‐optimizes their electronic states and lowering the energy barrier for water dissociation. Self‐powered H 2 production system can be achieved using Zn–H₂O batteries to drive anion exchange membrane water electrolysis cell, demonstrating its practicability.