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Active Interfacial Perimeter in Pt/CeO2 Catalysts with Embedding Structure for Water-Tolerant Toluene Combustion
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    Active Interfacial Perimeter in Pt/CeO2 Catalysts with Embedding Structure for Water-Tolerant Toluene Combustion
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    • Menglan Xiao
      Menglan Xiao
      Flavors and Fragrance Engineering and Technology Research Center of Henan Province, College of Tobacco Science, Henan Agricultural University, Zhengzhou 450046, P. R. China
      Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
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    • Dawei Han
      Dawei Han
      Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
      More by Dawei Han
    • Xueqin Yang
      Xueqin Yang
      College of Forestry, Henan Agricultural University, Zhengzhou 450002, P. R. China
      More by Xueqin Yang
    • Jing Yu
      Jing Yu
      Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
      More by Jing Yu
    • Bo Shi
      Bo Shi
      College of Chemistry and Materials Science, Hebei Key Laboratory of Inorganic Nano-materials, Hebei Normal University, Shijiazhuang 050024, P. R. China
      More by Bo Shi
    • Yucong Guo
      Yucong Guo
      Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
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    • Xiaolin Yu*
      Xiaolin Yu
      School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, P. R. China
      *Email: [email protected]
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    • Maofa Ge*
      Maofa Ge
      Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, P. R. China
      University of Chinese Academy of Sciences, Beijing 100049, P. R. China
      *Email: [email protected]
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    Other Access OptionsSupporting Information (1)

    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2024, 58, 51, 22808–22817
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    https://doi.org/10.1021/acs.est.4c06977
    Published December 9, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Supported Pt catalysts are often subjected to severe deactivation under the conditions of high temperature and water vapor in catalytic oxidation; thus, the superior stability and water-resistant ability of catalysts have great significance for the effective degradation of volatile organic compounds (VOCs). Herein, we constructed a Pt/CeO2-N catalyst with an active interfacial perimeter, in which Pt species were partially embedded in the defective CeO2-N support to prevent the sintering. A significant charge transfer between Pt species and ceria in the embedding structure occurred via the Pt-CeO2 interface, which induced the formation of a Pt4+-Ov-Ce3+ interfacial structure. Experimental research and theoretical calculations demonstrated that the active Pt4+-Ov-Ce3+ interface promoted the activation and migration of lattice oxygen, thus facilitating the participation of oxygen species in toluene oxidation. Consequently, Pt/CeO2-N showed excellent catalytic performance for toluene degradation. In situ DRIFTS and DFT calculation proved that the Pt4+-Ov-Ce3+ interfacial sites served as the intrinsic active center in the dissociation of H2O to generate ·OH, which contributed to the formation of benzaldehyde, thus remarkably improving the water-resistant property. This study provided a facile strategy for fabricating the interfacial embedding structure to enhance the catalytic activity and water tolerance for eliminating VOCs in practical application.

    Copyright © 2024 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.est.4c06977.

    • Catalyst characterization, catalytic activity test, and computational details; SEM images of supports and catalysts; Raman spectra and XPS results of supports; XRD patterns of all samples; nitrogen adsorption–desorption isotherms; pore-size distribution curves of samples; STEM-EDS elemental mappings of the Pt/CeO2-N sample; HAADF-STEM and HRTEM images of the Pt/CeO2 sample; Raman spectra of all samples; catalytic stability test over Pt/CeO2-N at 164 °C; formation energy of oxygen vacancy; intermediate MS signals in the toluene-TPD experiment; time-resolved in situ DRIFTS profiles under different conditions; corresponding contour projection of toluene transient reaction; textural parameters of all catalysts and the content of metals; catalytic performances of the as-prepared catalysts; quantification results of H2 consumption in H2-TPR; and quantification results of area integrals in O2-TPD (PDF)

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    Environmental Science & Technology

    Cite this: Environ. Sci. Technol. 2024, 58, 51, 22808–22817
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.est.4c06977
    Published December 9, 2024
    Copyright © 2024 American Chemical Society

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