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Ab Initio Investigation of CH4 Dehydrogenation on a (CeO2)10 Cluster

  • Carina S. T. Peraça
    Carina S. T. Peraça
    São Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, Brazil
    Department of Physics, Federal University of Pelotas, P.O. Box 354, 96010-900, Pelotas, RS, Brazil
  • Karla F. Andriani
    Karla F. Andriani
    Department of Biological Sciences, Federal University of Piauí, P.O. Box 64900-000, 64900-000 Bom Jesus, PI, Brazil
    São Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, Brazil
  • Maurício J. Piotrowski
    Maurício J. Piotrowski
    Department of Physics, Federal University of Pelotas, P.O. Box 354, 96010-900, Pelotas, RS, Brazil
  • , and 
  • Juarez L. F. Da Silva*
    Juarez L. F. Da Silva
    São Carlos Institute of Chemistry, University of São Paulo, P.O. Box 780, 13560-970, São Carlos, SP, Brazil
    *Email: [email protected]
Cite this: J. Phys. Chem. C 2022, 126, 29, 11937–11948
Publication Date (Web):July 15, 2022
https://doi.org/10.1021/acs.jpcc.2c02038
Copyright © 2022 American Chemical Society

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    Abstract

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    We report a theoretical investigation of the activation and dehydrogenation of CH4 on a (CeO2)10 cluster based on density functional theory calculations combined with the unity bond index-quadratic exponential potential approach. As expected, we identified a physisorption interaction mechanism between the CH4 and (CeO2)10 systems. Along the dehydrogenation, the interaction CHn–(CeO2)10 occurs by chemisorption via the formation of C–O and H–O bonds. Due to adsorption effects, the oxidation state of Ce atoms changes from Ce4+ to Ce3+, which results in the elongation of the Ce–O bonds due to the larger radius of the Ce3+ species, and hence, it affects the formation of the CO and CH3OH species. Our combined approach showed that the first dehydrogenation step involves a transition-state formation induced by the molecular hybridization before the CH3 radical formation. Finally, our results indicate trends for new compound formation, once the energy barrier involved in the first step of dehydrogenation is overcome.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpcc.2c02038.

    • Computational details and definitions about the structural, energetic, and electronic parameters for the adsorption properties of all calculated systems; information about the local magnetic moments of the Ce atoms for all reported configurations (PDF)

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    Cited By

    This article is cited by 1 publications.

    1. Pedro Ivo R. Moraes, Albert F. B. Bittencourt, Karla F. Andriani, Juarez L. F. Da Silva. Theoretical Insights into Methane Activation on Transition-Metal Single-Atom Catalysts Supported on the CeO2(111) Surface. The Journal of Physical Chemistry C 2023, 127 (33) , 16357-16366. https://doi.org/10.1021/acs.jpcc.3c02653

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