NIRT: Design of Nanoporous Molecular Square Catalysts using Multiscale Modeling

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AbstractProposal Title: NIRT: Design of Nanoporous Molecular Square Catalysts Using Multiscale ModelingProposal Number: CTS-0102612Principal Investigator:Randall SnurrInstitution: Northwestern UniversityThis proposal was submitted in response to the solicitation "Nanoscale Science and Engineering" (NSF 00-119). New multi-scale modeling approaches will be applied to novel nanoporous materials for selective oxidation catalysts. Linkages will be developed to permit the modeling of both physical processes and chemical interactions. State-of-the-art embedded cluster quantum chemical methods will be interfaced with iterative quantum/classical calculations. Continuum, atomistic, and quantum descriptions will be linked to yield a general description of the behavior of the reactive system Electronic information will be incorporated into the statistical mechanical simulations through a novel development of the Fukui function. Enhancement of microkinetic reaction modeling will be coupled with mass transfer effects. The multiscale model will be applied to new mesoporous "artificial enzymes," resembling molecular squares and composed of zinc porphyrin walls, rhenium corners, and a manganese porphyrin catalyst. Stable, nanoscale cavity environments will be synthesized and organized through self-assembly. Through the modeling effort new catalysts, based on these materials, will be designed. Model reactions to be studied are the epoxidations of olefins. This modeling work has the potential to guide the design of catalysts capable of mimicking biological processes and performing enantioselective syntheses.