Supported Rhodium Catalysts for Ammonia–Borane Hydrolysis: Dependence of the Catalytic Activity on the Highest Occupied State of the Single Rhodium Atoms
Liangbing Wang
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
These authors contributed equally to this work.
Search for more papers by this authorHongliang Li
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
These authors contributed equally to this work.
Search for more papers by this authorWenbo Zhang
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
Search for more papers by this authorXiao Zhao
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
Search for more papers by this authorJianxiang Qiu
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
Search for more papers by this authorAowen Li
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
Search for more papers by this authorXusheng Zheng
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
Search for more papers by this authorCorresponding Author
Prof. Zhenpeng Hu
School of Physics, Nankai University, Tianjin, 300071 P.R. China
Search for more papers by this authorCorresponding Author
Prof. Rui Si
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204 P.R. China
Search for more papers by this authorCorresponding Author
Prof. Jie Zeng
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
Search for more papers by this authorLiangbing Wang
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
These authors contributed equally to this work.
Search for more papers by this authorHongliang Li
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
These authors contributed equally to this work.
Search for more papers by this authorWenbo Zhang
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
Search for more papers by this authorXiao Zhao
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
Search for more papers by this authorJianxiang Qiu
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
Search for more papers by this authorAowen Li
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
Search for more papers by this authorXusheng Zheng
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
Search for more papers by this authorCorresponding Author
Prof. Zhenpeng Hu
School of Physics, Nankai University, Tianjin, 300071 P.R. China
Search for more papers by this authorCorresponding Author
Prof. Rui Si
Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204 P.R. China
Search for more papers by this authorCorresponding Author
Prof. Jie Zeng
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
Search for more papers by this authorGraphical Abstract
Phase-dependent: When a catalyst consisting of isolated rhodium atoms dispersed on the surface of VO2 nanorods was employed for ammonia–borane hydrolysis, the activation energy changed when the substrate underwent a phase transition. Mechanistic studies indicate that the catalytic performance depends directly on the highest occupied state of the single Rh atoms, which is determined by the band structure of the substrate.
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.
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