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It is a great challenge to induce the formation of the RuP4 phase and realize the construction of a metal‐rich phase/phosphorus‐rich phase‐ruthenium phosphide heterostructure by directional regulation of the proportion of P and metal atoms. The ultra‐high conductivity of Ru2P and the excellent ability of V‐doped RuP4 to absorb/desorb H* are confirmed by density functional theory (DFT) calculations, which laid a theoretical foundation for the construction of a unique Ru2P/V‐RuP4 structure to accelerate HER reaction kinetics. This work innovatively uses the V‐doping strategy to induce the formation of RuP4 phase with high intrinsic activity, and finally construct V‐RuxPy nanosheets with rich Ru/Ru2P/V‐RuP4 heterostructures. Thanks to the rich Ru/Ru2P/V‐RuP4 heterostructure and the optimization of V dopants, the V‐RuxPy catalyst only needs 180 mV to obtain an industrial‐grade current density of 1 A cm−2. In summary, this work provides a new idea for the design and performance optimization of ruthenium‐based catalysts. [ABSTRACT FROM AUTHOR]

Transition metal phosphide is regarded as one of the most promising candidates to replace noble‐metal hydrogen evolution reaction (HER) electrocatalysts. Nevertheless, the controllable design and synthesis of transition metal phosphide electrocatalysts with efficient and stable electrochemical performance are still very challenging. Herein, a novel hierarchical HER electrocatalyst consisting of three‐dimensional (3D) coral‐like Mn‐doped Co2P@an intermediate layer of Ni2P generated in situ by phosphorization on Ni foam (MnCoP/NiP/NF) is reported. Notably, both the incorporation of Mn and introduction of the Ni2P interlayer promote Co atoms to carry more electrons, which is beneficial to reduce the force of the Co−H bond and optimize the adsorption energy of hydrogen intermediate (|ΔGH*|), thereby making MnCoP/NiP/NF exhibit outstanding HER performance with onset overpotential and Tafel slope as low as 31.2 mV and 61 mV dec−1, respectively, in 1 m KOH electrolyte. [ABSTRACT FROM AUTHOR]