Deciphering Ball Milling Mechanochemistry via Molecular Simulations of Collision‐Driven and Liquid‐Assisted Reactivity

The direct study of mechanical activation events in ball milling mechanochemistry is, at present, not directly accessible experimentally, which prompted us to examine it by theoretical modelling. We use molecular dynamics simulations to describe mechanical activation by fragmentation of crystal particles down to individual atoms, ions and ion pairs, and monitor subsequent product formation and agglomeration under neat and liquid-assisted conditions. We demonstrate that a small amount of the liquid additive facilitated product formation, while too much of it destabilised the product by stabilising the reactants. Our approach provides a fresh and detailed view of mechanochemistry that could allow for its theoretical optimisation including the targeted choice of a catalyst and its loading.