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Transformation of Highly Stable Pt Single Sites on Defect Engineered Ceria into Robust Pt Clusters for Vehicle Emission Control

  • Wei Tan
    Wei Tan
    Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States
    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, School of Environment, Center of Modern Analysis, Nanjing University, Nanjing 210093, P. R. China
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  • Shaohua Xie
    Shaohua Xie
    Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States
    More by Shaohua Xie
  • Yandi Cai
    Yandi Cai
    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, School of Environment, Center of Modern Analysis, Nanjing University, Nanjing 210093, P. R. China
    More by Yandi Cai
  • Meiyu Wang
    Meiyu Wang
    College of Engineering and Applied Sciences, Nanjing University, Nanjing, 210093, P. R. China
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  • Shuohan Yu
    Shuohan Yu
    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, School of Environment, Center of Modern Analysis, Nanjing University, Nanjing 210093, P. R. China
    More by Shuohan Yu
  • Ke-Bin Low
    Ke-Bin Low
    BASF Corporation, Iselin, New Jersey 08830, United States
    More by Ke-Bin Low
  • Yuejin Li
    Yuejin Li
    BASF Corporation, Iselin, New Jersey 08830, United States
    More by Yuejin Li
  • Lu Ma
    Lu Ma
    National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United States
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  • Steven N. Ehrlich
    Steven N. Ehrlich
    National Synchrotron Light Source II (NSLS-II), Brookhaven National Laboratory, Upton, New York 11973, United States
  • Fei Gao*
    Fei Gao
    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, School of Environment, Center of Modern Analysis, Nanjing University, Nanjing 210093, P. R. China
    *(F.G.) [email protected]
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  • Lin Dong
    Lin Dong
    Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Jiangsu Key Laboratory of Vehicle Emissions Control, School of Environment, Center of Modern Analysis, Nanjing University, Nanjing 210093, P. R. China
    More by Lin Dong
  • , and 
  • Fudong Liu*
    Fudong Liu
    Department of Civil, Environmental, and Construction Engineering, Catalysis Cluster for Renewable Energy and Chemical Transformations (REACT), NanoScience Technology Center (NSTC), University of Central Florida, Orlando, Florida 32816, United States
    *(F.L.) [email protected]
    More by Fudong Liu
Cite this: Environ. Sci. Technol. 2021, 55, 18, 12607–12618
Publication Date (Web):September 8, 2021
https://doi.org/10.1021/acs.est.1c02853
Copyright © 2021 American Chemical Society
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Supporting Info (1)»

Abstract

Engineering surface defects on metal oxide supports could help promote the dispersion of active sites and catalytic performance of supported catalysts. Herein, a strategy of ZrO2 doping was proposed to create rich surface defects on CeO2 (CZO) and, with these defects, to improve Pt dispersion and enhance its affinity as single sites to the CZO support (Pt/CZO). The strongly anchored Pt single sites on CZO support were initially not efficient for catalytic oxidation of CO/C3H6. However, after a simple activation by H2 reduction, the catalytic oxidation performance over Pt/CZO catalyst was significantly boosted and better than Pt/CeO2. Pt/CZO catalyst also exhibited much higher thermal stability. The structural evolution of Pt active sites by H2 treatment was systematically investigated on aged Pt/CZO and Pt/CeO2 catalysts. With H2 reduction, ionic Pt single sites were transformed into active Pt clusters. Much smaller Pt clusters were created on CZO (ca. 1.2 nm) than on CeO2 (ca. 1.8 nm) due to stronger Pt-CeO2 interaction on aged Pt/CZO. Consequently, more exposed active Pt sites were obtained on the smaller clusters surrounded by more oxygen defects and Ce3+ species, which directly translated to the higher catalytic oxidation performance of activated Pt/CZO catalyst in vehicle emission control applications.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.1c02853.

  • XRD, EDS-mapping, Raman spectra, CO oxidation activity on Pt/CexZr1-xO2-a, HAADF-STEM images, XANES linear combination fitting results, EXAFS fitting curves in R-space, C3H6 oxidation activity, etc. (PDF)

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