Abstract
Hydrogen (H2) production from alkaline water electrocatalysis is economically appealing yet significantly hindered by the sluggish H2O adsorption and H* binding kinetics on active sites during hydrogen evolution reaction (HER). Herein, we interfacially immobilize Ru clusters on the hierarchical nickel nitride (Ru-Ni3N) nanosheet arrays via the filling of Ru3+ species into the metal vacancies of nickel hydroxide precursors and the subsequent controllable nitridation. The optimized Ru-Ni3N shows the outstanding HER performance, affording a 30-fold rise in the intrinsic activity of Ni sites, a outperforming-Pt/C overpotential at ≥ 125 mA cm−2 while remaining a robust stability. We further establish by a combined study of density functional theory (DFT) calculations with experimental analyses that long-range Ni sites around Ru sites act as active sites via the electron delocalization, remarkably weakening the H2O adsorption and H* binding barriers for enhancing the alkaline HER kinetics. Moreover, it also demonstrates an excellent pH-universal HER and overall water splitting performance.
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