TY - JOUR
T1 - Microkinetic Models with Interacting Adsorbates and Langmuir-Hinshelwood Steps
T2 - Solving the Master Equation on Small Periodic Tiles
AU - Ge, Jiankai
AU - Adams, Kevin C.
AU - Peters, Baron
N1 - Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/12/14
Y1 - 2023/12/14
N2 - 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).
AB - 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).
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U2 - 10.1021/acs.jpcc.3c07387
DO - 10.1021/acs.jpcc.3c07387
M3 - Article
AN - SCOPUS:85180099802
SN - 1932-7447
VL - 127
SP - 23687
EP - 23695
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 49
ER -