The unprecedented ability of computations
to probe atomic-level
details of catalytic systems holds immense promise for the fundamentals-based
bottom-up design of novel heterogeneous catalysts, which are at the
heart of the chemical and energy sectors of industry. Here, we critically
analyze recent advances in computational heterogeneous catalysis.
First, we will survey the progress in electronic structure methods
and atomistic catalyst models employed, which have enabled the catalysis
community to build increasingly intricate, realistic, and accurate
models of the active sites of supported transition-metal catalysts.
We then review developments in microkinetic modeling, specifically
mean-field microkinetic models and kinetic Monte Carlo simulations,
which bridge the gap between nanoscale computational insights and
macroscale experimental kinetics data with increasing fidelity. We
finally review the advancements in theoretical methods for accelerating
catalyst design and discovery. Throughout the review, we provide ample
examples of applications, discuss remaining challenges, and provide
our outlook for the near future.