Water electrolysis is an ideal way to obtain 'green hydrogen', but the core challenge of its commercial application is to develop advanced electrocatalysts that can work efficiently and stably under wide pH conditions. In this study, we innovatively constructed a Cu3P support with a unique pyramid-like crystal structure by controllable surface oxidation and phosphating treatment on the three-dimensional (3D) copper foam skeleton, and further loaded ruthenium (Ru) to form a Ru-Cu3P/CF self-supporting electrode to form a unique composite structure. Ampere-grade hydrogen evolution at full pH was achieved. Benefiting from the fast charge transport guaranteed by the 3D conductive network, and the electronic synergistic effect between Ru and Cu3P support. the as-prepared Ru-Cu3P/CF catalyst enables better catalytic performance than commercial Pt/C catalyst in the whole pH range. Under alkaline and acidic conditions, the overpotential required to drive hydrogen evolution reaction (HER) to current density of 1 A cm-2 is only 241.7 mV and 281.3 mV. At the same time, under the working condition, Ru-Cu3P/CF also inherits excellent HER performance, which realizes the efficient electrolysis of seawater to produce hydrogen and the ampere-grade hydrogen evolution at low voltage (1.79 V) on the integrated membrane electrode assembly. The performance of Ru-Cu3P/CF catalyst is significantly better than that of most reported Ru-based catalysts. This work provides a new idea for the design of integrated electrocatalysts with high performance and low noble metal loading.
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Hydrogen production by electrolysis of water is a key technology to achieve green hydrogen energy economy, but it relies on advanced catalyst materials with high efficiency, stability, and wide pH adaptability. In this study, Ni, Ru, and Pt ternary metals were embedded into nitrogen-doped hollow carbon spheres (NHCSs) by hydrothermal tandem heat treatment to form ternary supported metal nanoparticles with high dispersion and ultra-small particle size (~ 1.3 nm), which realized efficient hydrogen evolution from multi-scenario electrocatalytic water splitting. In the whole pH range, the performance of NiRuPt/NHCSs is better than that of commercial Pt/C catalyst, and the overpotentials under alkaline, neutral, and acidic conditions are as low as 15.5, 20.0, and 29.5 mV, respectively. Under industrial conditions, NiRuPt/NHCSs also have excellent hydrogen evolution reaction (HER) performance, achieving efficient electrolysis of seawater for hydrogen production, and achieving Ampere-level hydrogen production at low voltage (~ 1.76 V) on integrated membrane electrode assemblies. Density functional theory (DFT) calculations show that in the NiRuPt ternary metal, the Pt site is conducive to promoting the desorption of *H to form H2, the Ru site is conducive to promoting the capture of H2O, and the Ni site is conducive to promoting the dissociation of H2O. Therefore, the formed NiRuPt ternary metal synergistically promotes multi-scenario efficient electrolysis of water to produce hydrogen. This study provides a new idea for the design of multi-component metal/carbon-based composite catalysts, and promotes the development of non-noble metal/noble metal composite catalysts in hydrogen production by electrolysis of water.
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