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Elucidation of the Active Sites in Single-Atom Pd1/CeO2 Catalysts for Low-Temperature CO Oxidation

  • Dong Jiang
    Dong Jiang
    The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States
    More by Dong Jiang
  • Gang Wan
    Gang Wan
    SLAC National Accelerator Laboratory, Stanford University, 2575 Sand Hill Road, Menlo Park, California 94025, United States
    More by Gang Wan
  • Carlos E. García-Vargas
    Carlos E. García-Vargas
    The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States
  • Linze Li
    Linze Li
    Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
    More by Linze Li
  • Xavier Isidro Pereira-Hernández
    Xavier Isidro Pereira-Hernández
    The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States
  • Chongmin Wang
    Chongmin Wang
    Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
  • , and 
  • Yong Wang*
    Yong Wang
    The Gene and Linda Voiland School of Chemical Engineering and Bioengineering, Washington State University, Pullman, Washington 99164, United States
    Institute for Integrated Catalysis, Pacific Northwest National Laboratory, Richland, Washington 99354, United States
    *Email: [email protected]
    More by Yong Wang
Cite this: ACS Catal. 2020, 10, 19, 11356–11364
Publication Date (Web):August 20, 2020
https://doi.org/10.1021/acscatal.0c02480
Copyright © 2020 American Chemical Society
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Abstract

Supported precious metals with atomic dispersion are of great interest in catalysis due to their potentials in achieving maximum atom efficiency and unique reactivities. Herein, the active sites for low-temperature CO oxidation are elucidated over single-atom Pd1/CeO2 catalysts prepared via high-temperature atom trapping (AT). The increased oxygen vacancies on CeO2 surface induced by 800 °C air calcination result in decreased Pd–CeO2 coordinations, i.e., the coordination-unsaturated Pd2+ on CeO2. Light-off and light-out measurements coupled with CO-DRIFTS and X-ray absorption characterization confirm that these coordination-unsaturated Pd2+ on CeO2 are much more reactive than the fully coordinated counterpart, evidenced by a decrease of T90 (temperature to achieve 90% conversion) by ∼100 °C in CO oxidation at a gas hourly space velocity of 300 L g–1 h–1.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.0c02480.

  • Experimental details, XRD patterns, STEM images, EXAFS fitting, detailed in situ DRIFTS data, CO light-off and light-out measurements, time-on-stream measurements of CO oxidation, and kinetic studies (PDF)

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