Mean field model parameterization to recover coverage-dependent kinetics

Goswami, Anshuman; Schneider, William F.

doi:10.1016/j.jcat.2023.07.013

Mean field model parameterization to recover coverage-dependent kinetics

Journal Article · Wed Jul 26 00:00:00 EDT 2023 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2023.07.013· OSTI ID:1993707

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University of Notre Dame, IN (United States); University of Notre Dame
University of Notre Dame, IN (United States)

Lateral interactions between adsorbates introduce coverage dependence into adsorption energies and activation barriers of surface reactions. Lattice-based kinetic Monte Carlo (kMC) simulations can capture these interactions quantitatively but are laborious to parameterize and solve. Mean field models are more tractable, but protocols to construct and parameterize them are unclear. Here we explore the ability of a coverage-aware mean-field model to map to a lattice-kMC model of a generic two-step reaction network, including quasi-equilibrated adsorption and rate-limiting dissociation steps. We derive expressions for mean-field and coverage-dependent adsorption energies and dissociation barriers and parameterize against lattice-kMC predictions. We show that the parameterized mean-field rates correlate with ground truth lattice-kMC results across a wide range of reaction conditions and identify regions where the mean field fails. The mean field model similarly captures kMC-derived rate-order, Arrhenius and Sabatier plots at a greatly reduced computational cost. Further, the results provide guidance for parameterizing mean-field models, benchmarked against explicit lattice-based approaches for incorporating the influence of coverage effects.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); University of Notre Dame, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; SC0021107

OSTI ID:: 1993707

Alternate ID(s):: OSTI ID: 2000233

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 426; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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