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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

Abstract

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 VO2 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 NH3BH3 hydrolysis were rationally designed by adjusting their highest occupied states.

Phasenabhängig: Wenn einzelne Rh‐Atome auf der Oberfläche von VO2‐Nanostäben als Katalysator für die Hydrolyse von Ammoniak‐Boran verwendet werden, ändert sich die Aktivierungsenergie bei einer Phasenumwandlung des Substrats. Mechanistische Studien weisen darauf hin, dass die katalytische Aktivität vom höchsten besetzten Zustand der einzelnen Rh‐Atome abhängt, der von der Bandenstruktur des Substrats bestimmt wird.

Authors:   Liangbing Wang, Hongliang Li, Wenbo Zhang, Xiao Zhao, Jianxiang Qiu, Aowen Li, Xusheng Zheng, Zhenpeng Hu, Rui Si, Jie Zeng
Journal:   Angewandte Chemie
Year:   2017
Pages:   n/a
DOI:   10.1002/ange.201701089
Publication date:   30-Mar-2017
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