Highly Connective Interfacial Hydrogen‐Bond Network Accelerates Proton‐Coupled Electron Transfer for Hydrogen Evolution at Ampere‐Level Current

Precisely manipulating the interfacial microenvironment within the electrochemical double layer to enhance proton‐coupled electron transfer reaction efficiency during the hydrogen evolution reaction remains a fundamental challenge. Herein, we employ ab initio molecular dynamics simulations to reveal that introducing RuO 2 into PtRu significantly improves the connectivity of the interfacial hydrogen‐bond network. In situ electrochemical characterization and theoretical calculations demonstrate that RuO 2 enables a transition from 2‐coordinated hydrogen‐bonded water to 4‐coordinated hydrogen‐bonded water. Coupled with the optimal H* adsorption energy regulated by PtRu alloy synergism, these effects accelerate proton‐coupled electron transfer kinetics at high current densities. Notably, the PtRu‐RuO 2 ‐based anion exchange membrane water electrolysis achieves a current density of 500 mA cm −2 at just 1.68 V under alkaline conditions and operates stably for nearly 1000 h at an industrial‐scale current density of 1000 mA cm −2 . This work provides an atomic‐level insight for designing efficient alkaline hydrogen evolution reaction catalysts at ampere‐level current.