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

生物催化剂通常实现高度的对映体选择性和活性，这是通过活性位点内有机官能团的纳米级组织而实现的。 在合成非均相催化剂中实现同样的目标仍然是难以捉摸的。 因此，该建议的智力价值是通过控制纳米尺度上有机官能团的相关连接性和空间组织来合理设计和合成杂化有机-无机材料中的功能催化位点。 所得到的多相催化剂依赖于多功能机制，以促进特定的吸附和反应物活化催化。 该研究将利用最近成功的努力，在实现显着的速率增强碱催化剂的合成，其中一个酸基团的反应物吸附和活化与碱合作的催化剂。一个系统的调查将探讨当地的酸碱分离和固定化碱强度的影响，以及使用水溶剂环境的催化。 最后，提出了一个全面的方法，将这些材料的对映选择性反应能力。 研究活动广泛影响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-无机材料的催化。 对研究生和本科生的培训将特别注意招收女生和少数民族学生。 外联活动包括K-12组成部分，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.