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Supported Rhodium Catalysts for Ammonia–Borane Hydrolysis: Dependence of the Catalytic Activity on the Highest Occupied State of the Single Rhodium Atoms
Author(s) -
Wang Liangbing,
Li Hongliang,
Zhang Wenbo,
Zhao Xiao,
Qiu Jianxiang,
Li Aowen,
Zheng Xusheng,
Hu Zhenpeng,
Si Rui,
Zeng Jie
Publication year - 2017
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201701089
Subject(s) - ammonia borane , catalysis , rhodium , chemistry , metal , hydrolysis , nanorod , inorganic chemistry , ammonia , transition metal , noble metal , hydrogen production , materials science , nanotechnology , organic chemistry
Supported metal nanocrystals have exhibited remarkable catalytic performance in hydrogen generation reactions, which is influenced and even determined by their supports. Accordingly, it is of fundamental importance to determine the direct relationship between catalytic performance and metal–support interactions. Herein, we provide a quantitative profile for exploring metal–support interactions by considering the highest occupied state in single‐atom catalysts. The catalyst studied consisted of isolated Rh atoms dispersed on the surface of VO 2 nanorods. It was observed that the activation energy of ammonia–borane hydrolysis changed when the substrate underwent a phase transition. Mechanistic studies indicate that the catalytic performance depended directly on the highest occupied state of the single Rh atoms, which was determined by the band structure of the substrates. Other metal catalysts, even with non‐noble metals, that exhibited significant catalytic activity towards NH 3 BH 3 hydrolysis were rationally designed by adjusting their highest occupied states.