NIRT: Design of Nanoporous Molecular Square Catalysts using Multiscale Modeling

摘要提案题目：NIRT：基于多尺度模型的纳米多孔分子方剂催化剂设计提案号：cts -0102612项目负责人：Randall snurr机构：西北大学该提案应“纳米尺度科学与工程”（NSF 00-119）的征求而提交。新的多尺度建模方法将应用于新型纳米多孔材料的选择性氧化催化剂。将建立联系，以便对物理过程和化学相互作用进行建模。最先进的嵌入式簇量子化学方法将与迭代量子/经典计算相结合。连续体、原子和量子描述将被联系起来，以产生反应系统行为的一般描述。电子信息将通过福井函数的新发展被纳入统计力学模拟。微动力学反应模型的增强将与传质效应相结合。多尺度模型将应用于新型介孔“人工酶”，类似于分子正方形，由锌卟啉壁、铼角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来合成和组织。通过建模工作，基于这些材料的新型催化剂将被设计出来。要研究的模型反应是烯烃的环氧化反应。这项建模工作有可能指导设计能够模拟生物过程和进行对映选择性合成的催化剂。

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.