posted on 2023-12-04, 19:48authored byJiankai Ge, Kevin C. Adams, Baron Peters
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).