The objective of our research is to develop fundamental insight into small molecule activation in molecular complexes that will provide the basis for new approaches in rational catalyst design. Our focus is bi-functional � ambiphilic centers � molecular complexes comprised of both electron-rich and electron-poor sites, that provide an environment for heterolytic activation of molecular hydrogen and other small molecules such as CO2 for transformation to fuels for energy storage. We are using a wide array of theoretical tools in order to gain detailed understanding of the nature of the bonding and non-bonding interactions, and their different contributions to the reactivity of H2 in reactions catalyzed by Frustrated Lewis pairs. Our approach initially uses ab-initio calculations, bond orbital analysis and energy decomposition analysis, to study the molecular interactions in gas-phase and then widens to preform explicit solvent simulations using classical and QM/MM approaches for more realistic and accurate modeling of the reactions in condensed phase.  We will present our detailed analysis for Lutidine-BCl3 Lewis pair, comparing with our experimental results, and will describe our study of H2 activation and catalysis by intramolecular linked FLPs.

Understanding catalytic hydrogenation by Frustrated Lewis Pairs: Insight from theory and simulation

247th National Meeting (2014)

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