In the past decade, the use of first principles, periodic Density Functional Theory (DFT) calculations has emerged as central tool in the understanding and development of new heterogeneous catalysts.  While such calculations provide essential information about the energetics of elementary reactions, however, they have struggled to provide direct insights into the effect of liquid solvents on surface chemistry.  This consideration has been especially challenging for nanoporous zeolites, wherein confinement of the solvents in nanometer-scale pores, in addition to the interaction of the liquids with the catalytic active sites, introduces additional complexities to the catalytic processes.<br/>In this talk, recent efforts in our group to elucidate the structure of liquid water in the pores of zeolite Beta will be described.  We combine extensive ab-initio molecular dynamics (AIMD) simulations with quasi-harmonic determinations of the water entropy to produce comprehensive phase diagrams of water structure and stability.  The impact of catalytic active sites, such as silanol defects and framework substituted-transition metal ions, is rigorously analyzed, and the existence of both cluster-like and modified extended aqueous phases is demonstrated.  These results are interpreted in terms of the local structure and hydrogen bonding networks around the active sites.  Finally, the impact of these aqueous phenomena on elementary reactions that are often catalyzed by Lewis acid zeolites, including water activation and ethanol dehydration, is discussed, and perspectives for application of these techniques to a broader ensemble of catalytic processes are provided.<br/> <br/>

First principles studies of the impact of solvent structure on catalysis in nanoporous zeolites

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.