Synergy of Torsion Strained and Ligand Effect for Relay Acceleration of Industrial High‐pH Hydrogen Evolution

Abstract Noble metal Pt‐based catalysts have slow water dissociation kinetics at high pH conditions, making it difficult for water molecules to be electrochemically activated. Utilizing ligand effect and strain effect to tailor catalytic active sites is a common method, while the understanding of mechanism of their interaction remains obscure due to the complexity of the process. This study proposes a pulse‐induced torsional strained PtRu mesocrystals (PtRu MCs) with 20 times higher mass activity than commercial Pt/C. The combination of experimental results and theoretical calculations reveals that the ligand effect induced by Ru doping accelerates the kinetics of the water dissociation reaction, while the pulse‐induced torsion strained dominates the thermodynamic optimization of the hydrogen adsorption reaction. The structure‐activity relationship defined by the synergistic effect under the complementary advantages of the strain and doping provides guidance for the design of future basic hydrogen evolution catalysts. The catalyst can run stably at 1 A cm⁻² for 500 h, showing potential for industrial application.