Modulating Electronic Metal‐Support Interactions to Boost Visible‐Light‐Driven Hydrolysis of Ammonia Borane: Nickel‐Platinum Nanoparticles Supported on Phosphorus‐Doped Titania

Abstract Ammonia borane (AB) is a promising material for chemical H 2 storage owing to its high H 2 density (up to 19.6 wt %). However, the development of an efficient catalyst for driving H 2 evolution through AB hydrolysis remains challenging. Therefore, a visible‐light‐driven strategy for generating H 2 through AB hydrolysis was implemented in this study using Ni−Pt nanoparticles supported on phosphorus‐doped TiO 2 (Ni‐Pt/P‐TiO 2 ) as photocatalysts. Through surface engineering, P‐TiO 2 was prepared by phytic‐acid‐assisted phosphorization and then employed as an ideal support for immobilizing Ni−Pt nanoparticles via a facile co‐reduction strategy. Under visible‐light irradiation at 283 K, Ni 40 Pt 60 /P‐TiO 2 exhibited improved recyclability and a high turnover frequency of 967.8 mol mol Pt −1 min −1 . Characterization experiments and density functional theory calculations indicated that the enhanced performance of Ni 40 Pt 60 /P‐TiO 2 originated from a combination of the Ni−Pt alloying effect, the Mott–Schottky junction at the metal‐semiconductor interface, and strong metal‐support interactions. These findings not only underscore the benefits of utilizing multipronged effects to construct highly active AB‐hydrolyzing catalysts, but also pave a path toward designing high‐performance catalysts by surface engineering to modulate the electronic metal‐support interactions for other visible‐light‐induced reactions.