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，这是通过活性中心内有机官能团的纳米级组织实现的。在人工合成的多相催化剂中实现同样的目标仍然难以实现。因此，这一建议的智力价值在于通过控制有机官能团在纳米尺度上的相关连接性和空间组织，合理地设计和合成有机-无机杂化材料中的功能催化中心。由此产生的多相催化剂依赖于多功能机制来促进特定的吸附和催化反应的反应物活化。这项研究将利用最近成功的努力，通过合成酸性基团与碱协同作用的催化剂来显著提高碱催化的速度，以吸附和活化反应物。一项系统的研究将探索局部酸碱分离和固定化碱强度的影响，以及使用水介质环境进行催化。最后，提出了将对映选择性反应能力引入到这些材料中的综合方法。这些研究活动广泛影响了未来科学家在催化剂合成和表征方面的培训，重点是使用有机-无机杂化材料的催化。研究生和本科生的培养将特别重视招收女性和少数民族学生。外联活动包括K-12部分，以向中学生介绍化学工程的未来方向和挑战为主题。

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.