Predictive beyond-mean-field rate equations for multisite lattice–gas models of catalytic surface reactions: CO oxidation on Pd(100)

Liu, Da -Jiang; Zahariev, Federico; Gordon, Mark S.; Evans, James W.

doi:10.1021/acs.jpcc.6b10102

Title: Predictive beyond-mean-field rate equations for multisite lattice–gas models of catalytic surface reactions: CO oxidation on Pd(100)

Journal Article · Tue Nov 29 00:00:00 EST 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b10102· OSTI ID:1349905

Liu, Da -Jiang ^[1]; Zahariev, Federico ^[1]; Gordon, Mark S. ^[1]; Evans, James W. ^[1]

Ames Lab. and Iowa State Univ., Ames, IA (United States)

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. Furthermore, 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.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1349905

Report Number(s):: IS-J-9097

Journal Information:: Journal of Physical Chemistry. C, Vol. 120, Issue 50; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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