Fe Single Atoms Enable Lattice Compression and Schottky‐Like Interfaces for Efficient Hydrogen Evolution on Ru Nanoparticles

In the alkaline hydrogen evolution reaction (HER), the optimization of hydrogen binding energy (HBE) is generally constrained by the intrinsic trade‐off between water dissociation and hydrogen adsorption. Herein, we propose a dual‐regulation strategy that enables precise modulation of this trade‐off through the synergistic coupling of lattice strain and interfacial electronic rearrangement. We construct a Fe single‐atom dual‐anchored Ru‐based catalyst (Fe SA Ru NP P@NC), in which Fe atoms are simultaneously embedded within Ru nanoparticles, inducing ∼2.8% lattice compression, and anchored on N, P co‐doped carbon via Fe‐N 3 P 1 coordination, thereby forming a Ru NPs/Fe‐N 3 P 1 ‐C Schottky‐like interface. The lattice compression tunes the Ru d‐band center and weakens the overly strong adsorption of H * and OH * , while interfacial charge redistribution compensates for the electronic structure shift induced by lattice strain, enabling precise regulation of the Ru─H interaction. As a result, the catalyst delivers an outstanding HER performance in 1.0 m KOH, requiring only 22 mV overpotential to reach 10 mA cm −2 , significantly outperforming commercial Pt/C (37 mV). Both experimental and theoretical results demonstrate that the synergistic interplay between lattice strain and interfacial charge transfer promotes water polarization and dissociation, while optimizing adsorption energy matching along the reaction pathway, thereby markedly accelerating HER kinetics.