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Electronic Metal–Support Interactions in Single-Atom Catalysts

Authors

  • Pingping Hu,

    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
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    • These authors contributed equally to this work.

  • Zhiwei Huang,

    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
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    • These authors contributed equally to this work.

  • Dr. Zakariae Amghouz,

    1. Unidad de Microscopia Electrónica, Servicios-Científico Técnicos, Universidad de Oviedo-CINN, Oviedo, 33006 (Spain)
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    • These authors contributed equally to this work.

  • Prof. Michiel Makkee,

    1. Catalysis Engineering, Department of Chemical Engineering, Delft University of Technology, 2628 BL Delft (The Netherlands)
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  • Fei Xu,

    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
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  • Prof. Freek Kapteijn,

    1. Catalysis Engineering, Department of Chemical Engineering, Delft University of Technology, 2628 BL Delft (The Netherlands)
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  • Dr. Alla Dikhtiarenko,

    1. Catalysis Engineering, Department of Chemical Engineering, Delft University of Technology, 2628 BL Delft (The Netherlands)
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  • Yaxin Chen,

    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
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  • Dr. Xiao Gu,

    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
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  • Prof. Xingfu Tang

    Corresponding author
    1. Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)
    • Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China)===

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  • This work was financially supported by the NSFC (21277032), the NCET (120131), the SCAPC (201306), and the Netherlands–China exchange program (13CDP013). The XAS and SXRD measurements were conducted at the Shanghai Synchrotron Radiation Facility, Chinese Academy of Sciences. We acknowledge Bart van der Linden and Jorrit Posthuma de Boer for their assistance with the TAP experiments.

Abstract

The synthesis of single-atom catalysts and the control of the electronic properties of catalytic sites to arrive at superior catalysts is a major challenge in heterogeneous catalysis. A stable supported single-atom silver catalyst with a controllable electronic state was obtained by anti-Ostwald ripening. An electronic perturbation of the catalytic sites that is induced by a subtle change in the structure of the support has a strong influence on the intrinsic reactivity. The higher depletion of the 4d electronic state of the silver atoms causes stronger electronic metal–support interactions, which leads to easier reducibility and higher catalytic activity. These results may improve our understanding of the nature of electronic metal–support interactions and lead to structure–activity correlations.

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