Synergizing metal-support interactions and spatial confinement boosts dynamics of atomic nickel for hydrogenations.

Gu, Jian; Jian, Minzhen; Huang, Li; Sun, Zhihu; Li, Aowen; Pan, Yang; Yang, Jiuzhong; Wen, Wu; Zhou, Wu; Lin, Yue; Wang, Hui-Juan; Liu, Xinyu; Wang, Leilei; Shi, Xianxian; Huang, Xiaohui; Cao, Lina; Chen, Si; Zheng, Xusheng; Pan, Haibin; Zhu, Junfa; Wei, Shiqiang; Li, Wei-Xue; Lu, Junling

Gu, Jian; Jian, Minzhen; Huang, Li; Sun, Zhihu; Li, Aowen; Pan, Yang; Yang, Jiuzhong; Wen, Wu; Zhou, Wu; Lin, Yue; Wang, Hui-Juan; Liu, Xinyu; Wang, Leilei; Shi, Xianxian; Huang, Xiaohui; Cao, Lina; Chen, Si; Zheng, Xusheng; Pan, Haibin; Zhu, Junfa; Wei, Shiqiang; Li, Wei-Xue; Lu, Junling.

Afiliación

Gu J; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Jian M; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Huang L; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Sun Z; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Li A; School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, China.
Pan Y; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Yang J; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Wen W; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Zhou W; School of Physical Sciences and CAS Key Laboratory of Vacuum Physics, University of Chinese Academy of Sciences, Beijing, China.
Lin Y; CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, China.
Wang HJ; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Liu X; Experimental Center of Engineering and Materials Science, University of Science and Technology of China, Hefei, China.
Wang L; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Shi X; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Huang X; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Cao L; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Chen S; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Zheng X; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef
Pan H; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Zhu J; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Wei S; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
Li WX; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China. sqwei@ustc.edu.cn.
Lu J; Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemical Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hef

Nat Nanotechnol ; 16(10): 1141-1149, 2021 Oct.

Article en En | MEDLINE | ID: mdl-34312515

ABSTRACT

ABSTRACT

Atomically dispersed metal catalysts maximize atom efficiency and display unique catalytic properties compared with regular metal nanoparticles. However, achieving high reactivity while preserving high stability at appreciable loadings remains challenging. Here we solve the challenge by synergizing metal-support interactions and spatial confinement, which enables the fabrication of highly loaded atomic nickel (3.1 wt%) along with dense atomic copper grippers (8.1 wt%) on a graphitic carbon nitride support. For the semi-hydrogenation of acetylene in excess ethylene, the fabricated catalyst shows extraordinary catalytic performance in terms of activity, selectivity and stability-far superior to supported atomic nickel alone in the absence of a synergizing effect. Comprehensive characterization and theoretical calculations reveal that the active nickel site confined in two stable hydroxylated copper grippers dynamically changes by breaking the interfacial nickel-support bonds on reactant adsorption and making these bonds on product desorption. Such a dynamic effect confers high catalytic performance, providing an avenue to rationally design efficient, stable and highly loaded, yet atomically dispersed, catalysts.

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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nat Nanotechnol Año: 2021 Tipo del documento: Article