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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]

Currently, the construction of heterostructures to optimize electrocatalytic activities is a hot research topic, since there is still a certain gap between the electrocatalytic properties of these heterostructures and that of Pt/C. With this in mind, we utilized in‐situ vapor‐phase phosphorization‐sulfurization to obtain the CoP3/MoS2−Co0.75Mo3S3.75 (CoP/CoMoS, for short) heterostructure on carbon cloth (CC), which exhibits Pt‐like electrocatalytic performance and excellent stability in acid electrolyte. Activated by CoP3 active phase, the electronic configuration of CoMoS and the adsorption energy of H* (▵GH*) are greatly optimized. Meanwhile, the rapid oxidation of CoMoS phase can be effectively avoided under the protection of CoP3 layer. This work provides a reference for the design of heterostructures and their mechanism of action in electrocatalysis. [ABSTRACT FROM AUTHOR]

Rational construction of high‐efficiency and low‐cost catalysts is one of the most promising ways to produce hydrogen but remains a huge challenge. Herein, interface engineering and heteroatom doping were used to synthesize V‐doped sulfide/phosphide heterostructures on nickel foam (V‐Ni3S2/NixPy/NF) by phosphating treatment at low temperature. The incorporation of V can adjust the electronic structure of Ni3S2, expose more active sites, and protect the 3D structure of Ni foam from damage. Meanwhile, the heterogeneous interface formed between Ni3S2 and NixPy can provide abundant active sites and accelerate electron transfer. As a result, the V‐Ni3S2/NixPy/NF nanosheet catalyst exhibits outstanding activity in the hydrogen evolution reaction (HER) with an extremely low overpotential of 90 mV at a current density of 10 mA cm−2 and stable durability in alkaline solution, which exceeds those most of the previously reported Ni‐based materials. This work shows that rational design by interfacial engineering and metal‐atom incorporation has a significant influence for efficient hydrogen evolution. [ABSTRACT FROM AUTHOR]

Platinum (Pt)‐based compounds are the benchmarked catalysts for hydrogen evolution reaction (HER) but exhibit slow kinetics in alkaline environments. The *OH accumulation on Pt surface can block active sites, affecting proton reduction and water re‐adsorption. Alloying Ruthenium (Ru) with Pt sites can significantly modulate the adsorption and desorption of water dissociation intermediates. Choosing suitable supports and utilizing metal‐support interaction (MSI) is crucial for active site optimization. PtRu alloy anchored on tungsten oxide (WO3) with rich oxygen vacancies (OV) is prepared through an ultrafast microwave‐assisted approach. Benefiting from the coupling effects between alloying and MSI, PtRu/WO3‐OV exhibits exceptionally high HER activity. In 1 m KOH, 1 m KOH + seawater, and 0.5 m H2SO4, it requires ultralow overpotentials of 9, 26, and 6 mV to achieve 10 mA cm−2, respectively. The designed catalyst surpasses commercial Pt/C in mass activity and demonstrates considerable potential for intermittent energy integration. Density functional theory reveals that alloying Ru with Pt sites significantly reduces the energy barrier of dissociating *OH, modulating blockage on the surface and then promoting the overall alkaline HER process. This study offers insights into the rapid synthesis of non‐carbon supported catalysts with Pt site modulation for alkaline hydrogen generation. [ABSTRACT FROM AUTHOR]