Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202305371
Keywords
Ammonia Borane Hydrolysis; Hydrogen Evolution; Ni-Pt; P-TiO2; Strong Metal-Support Interactions; Surface Engineering
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In this study, Ni-Pt nanoparticles supported on phosphorus-doped TiO2 were used as visible-light-driven photocatalysts for generating hydrogen through ammonia borane hydrolysis. The Ni40Pt60/P-TiO2 catalyst exhibited improved recyclability and a high turnover frequency. The enhanced performance was attributed to the combination of the Ni-Pt alloying effect, the Mott-Schottky junction, and strong metal-support interactions.
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 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, Ni40Pt60/P-TiO2 exhibited improved recyclability and a high turnover frequency of 967.8 mol H2 ${{_{{\rm H}{_{2}}}}}$ mol(Pt)(-1) min(-1). Characterization experiments and density functional theory calculations indicated that the enhanced performance of Ni40Pt60/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.
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