Single‐Atom Doping Synergizes With Ni ₄ W Oxygen Pump Trigger Lattice Oxygen Regeneration Engineering to Achieve Enhanced LOM Mechanism

ABSTRACT Boosting lattice oxygen participation while addressing its slow regeneration is key to preparing highly efficient oxygen evolution reaction (OER) catalysts. Herein, an “oxygen pump trigger compensation” strategy to overcome such challenge is proposed. The coupling between a single‐atom Ru‐doping and Ni 4 W alloy interface engineering is highlighted to fabricate a novel Ru‐doped NiFe hydroxide/Ni 4 W alloy heterojunction electrocatalyst (Ru‐NLW/NF) grown on nickel foam (NF) for accelerating the alkaline hydrogen evolution reaction (HER) and OER. High‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) and mechanism investigations reveal that atomically dispersed Ru single‐atom species enhance M d‐O p orbital hybridization, thereby accelerating direct lattice‐oxygen coupling. Ru‐induced lattice oxygen activation process is sustained by the Ni 4 W alloy, functioning as an “oxygen pump” that dynamically balances lattice oxygen regeneration and activity enhancement through the continuous supply of oxygen‐containing intermediates and electrons to NiFe hydroxide. As expected, the Ru‐NLW/NF modified with single atoms exhibits excellent electrochemical performance. HER and OER achieve 10 mA cm −2 at 159 mV and 180 mV, and display superior durability exceeding 100 h even at high current densities. By coupling single‐atom active sites with an oxygen‐pump mechanism, the catalyst synchronizes lattice‐oxygen participation and facile regeneration, yielding bifunctional catalysts with high activity and durability.