Interface Local‐Alkalinity Engineering for Enhanced Dehydrogenation Catalysis in Neutral Media

ABSTRACT Hydrous hydrazine has emerged as a promising liquid‐phase hydrogen storage material, but its practical application has long been constrained by sluggish reaction kinetics under neutral conditions. Drawing inspiration from interfacial engineering, we designed a NiPt‐Ni(OH) 2 interface that regulates the local microenvironment, enabling highly efficient hydrogen production from hydrous hydrazine under neutral conditions at room temperature. At the interfaces, strong electronic coupling is established and the adsorption of hydrazine is also altered. The resulting NiPt‐Ni(OH) 2 catalyst achieves a remarkable apparent turnover frequency of 310.7 h −1 at 298 K, representing the highest performance reported to date for hydrous hydrazine dehydrogenation without external base added during catalysis. Combined spectroscopic analysis and density functional theory calculations reveal that the interfacial Ni(OH) 2 not only donates electrons to the NiPt alloy, modulating its electronic structure but also provides Brønsted basic sites that promote a favorable linear adsorption configuration of hydrazine. This dual electronic and chemical modulation lowers the energy barrier for dehydrogenation and accelerates hydrogen evolution kinetics. Our findings establish a generalizable interface engineering paradigm for catalytic enhancement under mild conditions without relying on external alkaline additives.