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Nat Commun. 2019 Jan 16;10(1):234. doi: 10.1038/s41467-018-08136-3.

Non defect-stabilized thermally stable single-atom catalyst.

Author information

1
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
2
Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials, School of Materials, Tianjin University of Technology, Tianjin, 300384, China.
3
Department of Chemistry & Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education, Tsinghua University, Beijing, 100084, China.
4
Synchrotron Radiation Laboratory, Laser and Synchrotron Research Center (LASOR), The Institute for Solid State Physics, The University of Tokyo, 1-490-2 Kouto, Shingu-cho Tatsuno, Hyogo, 679-5165, Japan.
5
University of Chinese Academy of Sciences, Beijing, 100049, China.
6
School of Science, Royal Melbourne Institute of Technology University, Melbourne, VIC3001, Australia.
7
Synchrotron Radiation Nanotechnology Center, University of Hyogo, 1-490-2 Kouto, Shingu-cho Tatsuno, Hyogo, 679-5165, Japan.
8
Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials, School of Materials, Tianjin University of Technology, Tianjin, 300384, China. jluo@tjut.edu.cn.
9
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China. bqiao@dicp.ac.cn.
10
Dalian National Laboratory for Clean Energy, Dalian, 116023, China. bqiao@dicp.ac.cn.
11
Department of Chemistry & Key Laboratory of Organic Optoelectronics and Molecular Engineering of the Ministry of Education, Tsinghua University, Beijing, 100084, China. junli@tsinghua.edu.cn.
12
Department of Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China. junli@tsinghua.edu.cn.

Abstract

Surface-supported isolated atoms in single-atom catalysts (SACs) are usually stabilized by diverse defects. The fabrication of high-metal-loading and thermally stable SACs remains a formidable challenge due to the difficulty of creating high densities of underpinning stable defects. Here we report that isolated Pt atoms can be stabilized through a strong covalent metal-support interaction (CMSI) that is not associated with support defects, yielding a high-loading and thermally stable SAC by trapping either the already deposited Pt atoms or the PtO2 units vaporized from nanoparticles during high-temperature calcination. Experimental and computational modeling studies reveal that iron oxide reducibility is crucial to anchor isolated Pt atoms. The resulting high concentrations of single atoms enable specific activities far exceeding those of conventional nanoparticle catalysts. This non defect-stabilization strategy can be extended to non-reducible supports by simply doping with iron oxide, thus paving a new way for constructing high-loading SACs for diverse industrially important catalytic reactions.

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