The Design and Synthesis of Hybrid Organic-Inorganic Materials as Base Catalysts

生物催化剂通常具有高度的对映选择性和活性，这是通过活性位点内纳米级有机官能团的组织而实现的。在合成多相催化剂中实现同样的目标仍然是难以捉摸的。因此，本课题的智力优势在于通过在纳米尺度上控制有机官能团的相关连通性和空间组织，合理设计和合成有机-无机杂化材料中的功能催化位点。所得到的多相催化剂依赖于促进特定吸附和反应物活化的多功能机制进行催化。该研究将利用最近成功的研究成果，通过合成酸基与碱协同作用以吸附和活化反应物的催化剂，显著提高碱催化的速率。系统的研究将探讨局部酸碱分离和固定化碱强度的影响，以及使用水溶剂环境进行催化。最后，提出了一种将对映选择性反应能力纳入这些材料的综合方法。这些研究活动广泛地影响着未来科学家在催化剂合成和表征方面的培训，重点是使用混合有机-无机材料进行催化。研究生和本科生的培训将特别注意招收女性和少数民族学生。拓展活动包括K-12部分，以研究报告的形式向中学生介绍化学工程的未来方向和挑战。

Biological catalysts routinely achieve high degrees of enantioselectivity and activity, which is made possible via the nanoscale organization of organic functional groups within the active site. Achieving the same in synthetic heterogeneous catalysts has remained elusive. Accordingly, the intellectual merit of this proposal is to rationally design and synthesize functional catalytic sites in hybrid organic-inorganic materials via the control of relevant connectivity and spacial organization of organic functional groups on the nanoscale. The resulting heterogeneous catalysts rely on multifunctional mechanisms for facilitating specific adsorption and reactant activation for catalysis. The research will exploit recent successful efforts in achieving significant rate enhancements in base catalysis by the synthesis of catalysts in which an acid group acts cooperatively with base for reactant adsorption and activation. A systematic investigation will explore the effects of local acid-base separation and immobilized base strength, as well as the use of aqueous solvent environments for catalysis. Finally, a comprehensive approach for the incorporation of enantioselective reaction capability into these materials is proposed. The research activities broadly impact the training of future scientists in catalyst synthesis and characterization, with emphasis on catalysis using hybrid organic-inorganic materials. The training of graduate and undergraduate students will have special attention placed on the recruitment of female and minority students. Outreach activities include a K-12 component, in the form of research presentations to middle-school students on the topic of future directions and challenges in chemical engineering.