Articles producció científica> Enginyeria Química

Dimethyl carbonate synthesis from CO2 and methanol over CeO2: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism

  • Identification data

    Identifier: imarina:9381248
    Handle: https://hdl.handle.net/20.500.11797/imarina9381248
    Authors:
    Stoian DSugiyama TBansode AMedina Fvan Beek WHasegawa JYNakayama AUrakawa A
    Abstract:
    Surface intermediate species and oxygen vacancy-assisted mechanism over CeO2 catalyst in the direct dimethyl carbonate (DMC) synthesis from carbon dioxide and methanol are suggested by means of transient spectroscopic methodologies in conjunction with multivariate spectral analysis. How the two reactants, i.e. CO2 and methanol, interact with the CeO2 surface and how they form decisive surface intermediates leading to DMC are unraveled by DFT-based molecular dynamics simulation by precise statistical sampling of various configurations of surface states and intermediates. The atomistic simulations and uncovered stability of different intermediate states perfectly explain the unique DMC formation profile experimentally observed upon transient operations, strongly supporting the proposed oxygen vacancy-assisted reaction mechanism.

  • Others:

    Author, as appears in the article.: Stoian D; Sugiyama T; Bansode A; Medina F; van Beek W; Hasegawa JY; Nakayama A; Urakawa A
    Department: Enginyeria Química
    URV's Author/s: Medina Cabello, Francisco / STOIAN, DRAGOS CONSTANTIN
    Abstract: Surface intermediate species and oxygen vacancy-assisted mechanism over CeO2 catalyst in the direct dimethyl carbonate (DMC) synthesis from carbon dioxide and methanol are suggested by means of transient spectroscopic methodologies in conjunction with multivariate spectral analysis. How the two reactants, i.e. CO2 and methanol, interact with the CeO2 surface and how they form decisive surface intermediates leading to DMC are unraveled by DFT-based molecular dynamics simulation by precise statistical sampling of various configurations of surface states and intermediates. The atomistic simulations and uncovered stability of different intermediate states perfectly explain the unique DMC formation profile experimentally observed upon transient operations, strongly supporting the proposed oxygen vacancy-assisted reaction mechanism.
    Thematic Areas: Astronomia / física Chemistry (all) Chemistry (miscellaneous) Chemistry, multidisciplinary Ciências biológicas i Ciências biológicas iii Farmacia General chemistry Interdisciplinar Materiais Química
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: francesc.medina@urv.cat
    Author identifier: 0000-0002-3111-1542
    Record's date: 2024-10-12
    Papper version: info:eu-repo/semantics/publishedVersion
    Papper original source: Chemical Science. 14 (47): 13908-13914
    APA: Stoian D; Sugiyama T; Bansode A; Medina F; van Beek W; Hasegawa JY; Nakayama A; Urakawa A (2023). Dimethyl carbonate synthesis from CO2 and methanol over CeO2: elucidating the surface intermediates and oxygen vacancy-assisted reaction mechanism. Chemical Science, 14(47), 13908-13914. DOI: 10.1039/d3sc04466a
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2023
    Publication Type: Journal Publications

  • Keywords:

    Chemistry (Miscellaneous),Chemistry, Multidisciplinary
    Astronomia / física
    Chemistry (all)
    Chemistry (miscellaneous)
    Chemistry, multidisciplinary
    Ciências biológicas i
    Ciências biológicas iii
    Farmacia
    General chemistry
    Interdisciplinar
    Materiais
    Química

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