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Developing efficient and stable electrocatalysts for hydrogen evolution reaction (HER) over a wide pH range and industrial large‐scale hydrogen production is critical and challenging. Here, a tailoring strategy is developed to fabricate an outstanding HER catalyst in both acidic and alkaline electrolytes containing high‐density atomically dispersed Ru sites anchored in the CoP nanoparticles supported on carbon spheres (NC@RuSA‐CoP). The obtained NC@RuSA‐CoP catalyst exhibits excellent HER performance with overpotentials of only 15 and 13 mV at 10 mA cm−2 in 1 m KOH and 0.5 m H2SO4, respectively. The experimental results and theoretical calculations indicate that the strong interaction between the Ru site and the CoP can effectively optimize the electronic structure of Ru sites to reduce the hydrogen binding energy and the water dissociation energy barrier. The constructed alkaline anion exchange membrane water electrolyze (AAEMWE) demonstrates remarkable durability and an industrial‐level current density of 1560 mA cm−2 at 1.8 V. This strategy provides a new perspective on the design of Ru‐based electrocatalysts with suitable intermediate adsorption strengths and paves the way for the development of highly active electrocatalysts for industrial‐scale hydrogen production.

A 2D covalent organometallic nanosheet (COMS-Co) was synthesized through the one-step conjunction of sandwich coordinate motif with covalent heterocyclic linkage via the condensation of boronic acid, and it showed promising semiconducting properties.

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