Synergistic Manipulating Electron Buffer and Hydrogen Spillover of Pt Catalysts for Ampere‐Level Efficient and Durable Hydrogen Evolution

Developing ampere‐level efficient and durable alkaline hydrogen evolution reaction (HER) electrocatalysts is crucial yet challenging due to the excessive *H coverage, electrochemical etching, and mechanical exfoliation under extremely high bias voltage. Herein, we integrate electronic buffers and hydrogen spillover engineering to facilitate hydrogen production on industrial scale via in situ grown dense‐interface NiPt δ+ /Pt–NiO on foam nickel substrate. The tight riveting NiPt δ+ /Pt–NiO and shared Ni atom with substrate effectively prevent the aggregation and mechanical exfoliation of Pt at high current. Meanwhile, the formative high‐valent platinum (Pt δ+ ) due to built‐in electric field between NiPt and Pt–NiO as electronic buffer to capturing the electrons from adsorbed hydrogen (*H) through yielded anti‐bonding empty orbitals, preserving the Pt─Pt bond energy and electrochemical stability under HER potentials. Simultaneously, Pt δ+ weakens *H adsorption to trigger hydrogen spillover effect, which significantly enhancing H transfer kinetics. Consequently, the NiPt δ+ /Pt–NiO achieves record‐low overpotential of 5.5 and 191 mV at 10 and 1000 mA cm −2 , respectively, and is capable of running steadily for 1000 h at 1000 mA cm −2 . Furthermore, a membrane electrode assembly utilizing NiPt δ+ /Pt–NiO catalysts as cathode requires 1.78 V at 1000 mA cm −2 , and can operate stably for more than 500 h.