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Electron-Hopping Brings Lattice Strain and High Catalytic Activity in the Low-Temperature Oxidative Coupling of Methane in an Electric Field

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    Electron-Hopping Brings Lattice Strain and High Catalytic Activity in the Low-Temperature Oxidative Coupling of Methane in an Electric Field
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    † †Department of Applied Chemistry and §Department of Chemistry and Biochemistry, Waseda University, 3-4-1, Okubo, Shinjuku, Tokyo, 169-8555 Japan
    ‡ PRESTO, Japan Science and Technology Agency (JST), 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
    ∥ Center for Green Research on Energy and Environmental Materials, National Institute for Materials Science, 1-1, Namiki, Tsukuba, Ibaraki 305-0044, Japan
    *E-mail: [email protected]
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2018, 122, 4, 2089–2096
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    https://doi.org/10.1021/acs.jpcc.7b08994
    Published January 22, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Detailed reaction mechanisms for the oxidative coupling of methane (OCM) over Ce2(WO4)3 catalysts at low temperatures in an electric field were investigated. The influence of Ce cations in the Ce2(WO4)3 catalyst was evaluated by comparing the OCM activity over various Ln2(WO4)3 (Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, and Dy) catalysts in an electric field. The electronic states of Ln and W cations and the relationship between the distorted Ce2(WO4)3 structure and methane activation were examined using X-ray absorption fine structure (XAFS) measurements and first-principles calculations. The results reveal that the Ln2(WO4)3 catalysts with redox-active Ln cations (Ce, Pr, Sm, Eu, and Tb) show OCM activity. First-principles calculations indicate that Ce3+ species in the Ce2(WO4)3 structure are oxidized to Ce4+ species in an electric field by extracting electrons from the Ce 4f orbitals near the Fermi level; as a result, its structure is distorted. The results indicate that the redox reaction of Ln cations in Ln2(WO4)3 induced by an electric field brings lattice strain and a high OCM activity in an electric field.

    Copyright © 2018 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.7b08994.

    • Details of preparation procedures of the catalysts. Schematic diagrams of the reactor for activity tests (Figure S1) and in situ XAFS (Figure S2). Results of activity tests (Table S1). Results of various characterizations using XRD (Figure S3), XANES (Figure S4–S6), and N2 physisorption (Table S2). Calculated DOS (Figures S7–S10), band gaps (Tables S3 and S4), and bond lengths (Table S5). Results of Bader charge analyses (Table S6). Configuration of oxygen in Ln2(WO4)3 (Figure S11). Structure model of Ce2(WO4)3 (Figure S12). Charge density difference plots (Figures S13–S17) (PDF)

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    Cite this: J. Phys. Chem. C 2018, 122, 4, 2089–2096
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.7b08994
    Published January 22, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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