title: 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 VO2nanorods. 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 NH3BH3hydrolysis were rationally designed by adjusting their highest occupied states.
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Liangbing
authors.initials: L
authors.lastname: Wang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Hongliang
authors.initials: H
authors.lastname: Li
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Wenbo
authors.initials: W
authors.lastname: Zhang
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Xiao
authors.initials: X
authors.lastname: Zhao
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Jianxiang
authors.initials: J
authors.lastname: Qiu
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Aowen
authors.initials: A
authors.lastname: Li
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Xusheng
authors.initials: X
authors.lastname: Zheng
authors.affiliation: School of Physics, Nankai University, Tianjin, 300071, P.R. China.
authors.forename: Zhenpeng
authors.initials: Z
authors.lastname: Hu
authors.affiliation: Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, P.R. China.
authors.forename: Rui
authors.initials: R
authors.lastname: Si
authors.affiliation: Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P.R. China.
authors.forename: Jie
authors.initials: J
authors.lastname: Zeng
keywords: hydrolysis; metal-support interactions; rhodium; single-atom catalysts; vanadium dioxide