NIRT: Design of Nanoporous Molecular Square Catalysts using Multiscale Modeling

摘要提案标题：NIRT：利用多尺度模型设计纳米多孔分子方形催化剂提案编号：CTS-0102612主要研究员：Randall Snurr机构：西北大学本提案是响应“纳米科学与工程”（NSF 00-119）的征集而提交的。 新的多尺度建模方法将被应用于新型选择性氧化催化剂的纳米多孔材料。 将建立联系，以便对物理过程和化学相互作用进行建模。 国家的最先进的嵌入式集群量子化学方法将与迭代量子/经典计算接口。 连续统、原子论和量子论的描述将被联系起来，以产生对反应系统行为的一般描述 电子信息将被纳入统计力学模拟通过一个新的发展的福井功能。 微观动力学反应模型的增强将与传质效应相结合。 多尺度模型将被应用于新的介孔“人造酶”，类似于分子广场，由锌卟啉壁，角隅和锰卟啉催化剂组成。 稳定的纳米级空腔环境将通过自组装合成和组织。 通过建模工作，将设计基于这些材料的新催化剂。 要研究的模型反应是烯烃的环氧化反应。这种建模工作有可能指导催化剂的设计，能够模仿生物过程和进行对映选择性合成。

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.