Microkinetic Models with Interacting Adsorbates and Langmuir-Hinshelwood Steps: Solving the Master Equation on Small Periodic Tiles

Jiankai Ge, Kevin C. Adams, Baron Peters

Research output: Contribution to journalArticlepeer-review

Abstract

The most prevalent microkinetic modeling (MKM) techniques in catalysis assume mean-field coverages and noninteracting adsorbates (MF-MKMs) or use kinetic Monte Carlo (KMC) to explicitly track surface reactions on large numbers of sites. Between these extremes are models with mean-field adsorbate interactions, models with coverage-dependent adsorption and reaction energies, and models that invoke closures and truncations to account for correlated adsorbate positions. Using KMC results as a benchmark, we show that tilings corresponding to square and hexagonal lattices yield easily formulated, easily solved, and surprisingly accurate microkinetic models, even with interacting adsorbates and Langmuir-Hinshelwood steps. We demonstrate the MKM construction for the reaction 2A(g) ↔ 2A* → A2(g) on a square lattice (with Greek cross tiling) and on a hexagonal lattice (with new “creamcups” tiling).

Original languageEnglish (US)
Pages (from-to)23687-23695
Number of pages9
JournalJournal of Physical Chemistry C
Volume127
Issue number49
DOIs
StatePublished - Dec 14 2023

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Energy
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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