Using a combination of QM/MM, QM/MM and statstical mechanics, we explore the stability and reactivity of MOF structures, focusing specifically on the acid-gas stability of zeolitic imidazolate frameworks. We find several important cases where standard periodic density functinoal theory yields substantial errors as compared to carefully constructed QM/MM and QM/MM models utilizing "gold standard" coupled cluster theory. We later leverage these models in conjunction with a further statistical mechanics-based model that explains the unique acid gas stability of ZIF-71 observed in recent experiments.

Accurate and efficient computational studies of MOF stabiltiy and reactivity via QM/MM and QM/QM methods

ACS Spring 2022

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