Understanding the nature of active centers is critical for advancing catalysis. On many occasions, active centers are formed under operating conditions and are largely affected by the environment. Hence, our ability to model a catalytic process, compare with experimental measurements or make accurate prediction strongly depends on our knowledge of what the active site is. Quantum mechanical calculations are essential for obtaining quantitative energy descriptors or benchmarking extended models. An accurate representation of extended reactive systems, including solvents, flexible ligands, or confinement, gives rise to large ensembles of minima and anharmonic effects that result in large entropic changes. In this paper, I will briefly summarize the computational approaches necessary to obtain an integrated multiscale picture of reactivity and transport at the atomistic level. I will discuss a swarm-intelligence algorithm that can efficiently locate a number of minima even for large systems (~10<sup>2</sup>-10<sup>3</sup> atoms) and show how it can be applied to catalysis-relevant problems. I will also discuss the genesis of anharmonic effects as a result of solvents and how one can quantitatively recover the entropic contributions from large-scale with enhanced sampling simulations. I will close with the outlook of how statistical mechanics and data science tools can be leveraged to enable new discoveries.

Tackling entropy in catalysis: Global optimizers, large scale simulations and enhanced sampling

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ACS Spring 2023

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