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

Ammonia borane (AB) is a promising material for chemical H₂ storage owing to its high H₂ density (up to 19.6 wt %). However, the development of an efficient catalyst for driving H₂ evolution through AB hydrolysis remains challenging. Therefore, a visible-light-driven strategy for generating H₂ through AB hydrolysis was implemented in this study using Ni-Pt nanoparticles supported on phosphorus-doped TiO₂ (Ni-Pt/P-TiO₂ ) as photocatalysts. Through surface engineering, P-TiO₂ 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, Ni₄₀ Pt₆₀ /P-TiO₂ exhibited improved recyclability and a high turnover frequency of 967.8 mol H 2 _ H₂ molPt ⁻¹ min⁻¹ . Characterization experiments and density functional theory calculations indicated that the enhanced performance of Ni₄₀ Pt₆₀ /P-TiO₂ 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.