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Predictive Beyond-Mean-Field Rate Equations for Multisite Lattice–Gas Models of Catalytic Surface Reactions: CO Oxidation on Pd(100)

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    Predictive Beyond-Mean-Field Rate Equations for Multisite Lattice–Gas Models of Catalytic Surface Reactions: CO Oxidation on Pd(100)
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    † § ∥ †Ames Laboratory − USDOE, ‡Department of Chemistry, §Department of Mathematics, and ∥Department of Physics & Astronomy, Iowa State University, Ames, Iowa 50011, United States
    *D.-J. Liu. E-mail: [email protected]
    *J. W. Evans. E-mail: [email protected]
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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2016, 120, 50, 28639–28653
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    https://doi.org/10.1021/acs.jpcc.6b10102
    Published November 29, 2016
    Copyright © 2016 American Chemical Society
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    Abstract

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    Tailored multisite lattice–gas (msLG) models are developed for CO oxidation on Pd(100) at low-pressures. These models include multiple adsorption site types and superlattice adlayer ordering due to short-range exclusion for highly mobile reactant adspecies. However, they are simplified to neglect longer-range weaker adspecies interactions, so that the key energetic parameters are the CO desorption barrier and the reaction barrier. We discuss existing density functional theory results for these energies and present additional analysis for CO adsorption. After also including an appropriate nontrivial specification of the dynamics of adsorption onto mixed reactant adlayers, we develop rate equations for the reaction kinetics. Our formulation goes beyond traditional mean-field (MF) Langmuirian treatments by accounting for multiple adsorption sites and for the strong spatial correlations associated with superlattice ordering. Specifically, we utilize factorization approximations based on appropriate site motifs, and also Padé resummation of exact low-coverage expansions for sticking coefficients. Our beyond-MF rate equations are successful in accurately predicting key aspects of reactive steady-state behavior, and thus expand the utility of rate equation formulations in surface chemistry. This is confirmed by comparison with precise kinetic Monte Carlo simulation results. Specifically, we not only assess bistability and criticality observed for CO oxidation but also find more complex multistability associated with symmetry-breaking transitions in high-coverage CO adlayers.

    Copyright © 2016 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.6b10102.

    • Cluster geometries for analysis of CO adsorption at br sites (S1); additional plane-wave DFT VASP analysis (S2); results for various levels of theory with localized atomic bases for CO+8Pd (S3); additional results with unrestricted spin for PBE and PBE0 (S4); modifications to the model of Hoffmann et al. producing MF-type bistability (S5) (PDF)

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    Cited By

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    This article is cited by 17 publications.

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    The Journal of Physical Chemistry C

    Cite this: J. Phys. Chem. C 2016, 120, 50, 28639–28653
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpcc.6b10102
    Published November 29, 2016
    Copyright © 2016 American Chemical Society
    Request reuse permissions

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