Investigative and developmental catalysis: polymer electrolyte fuel cells, asymmetric catalysis and reusable polymer-catalyst frameworks

我们的主要目标是开发高效、绿色和新的催化反应来合成药物、杀虫剂，并在燃料电池中产生能量。我们通过研究催化剂的工作原理，并利用这些信息来指导制备更好的催化剂和反应，从而最大限度地提高催化剂的反应性、寿命和可重用性。我们制备活性的溶解催化剂、高度可重复使用的固体聚合物催化剂骨架和定制的纳米颗粒。我们已经制备和研究了重要的和广泛使用的Noyori酮加氢反应中的大多数中间体。从这项研究中，我们了解到如何开发一种系统，在非常温和的条件下氢化酯来制造醇。目前，将酯转化为醇的工业转化需要大量易燃的固体氢化物试剂，这些试剂处理起来很危险，而且会产生废物。酯加氢是一种绿色、高效、可替代的技术。药物是复杂的分子。制备它们的最有效的方法是从简单的制备、廉价的具有内在复杂性的分子开始。从我们的研究中，我们了解到如何开发一种新的反应，即单氢化亚胺的去对称化。这个反应使在一个催化步骤中获得的有用的分子复杂性增加了五倍。我们还构建了催化剂--目前只用一次就丢弃的普通催化剂的有机骨架。我们的骨架是迄今为止氢化和环异构化反应中最可重复使用的手性催化剂。我们的目标是准备连续流动塔反应器，原料进入顶部，产品从底部出来。

Our primary objective is to develop efficient, green, and new catalytic reactions to synthesize pharmaceuticals, insecticides, and to produce energy in fuel cells. We maximize the reactivity, lifetime, and reusability of our catalysts by studying how they work, and using this information to guide the preparation of better catalysts and reactions. We prepare active dissolved catalysts, highly reusable solid polymer-catalyst frameworks, and tailored nanoparticles. We have prepared and studied most intermediates in the important, and widely-used Noyori ketone hydrogenation. From this study, we learned how to develop a system that hydrogenates esters to make alcohols under remarkably mild conditions. The industrial conversion of esters to alcohols presently requires large amounts of flammable solid hydride reagents that are dangerous to handle and that create waste. Ester hydrogenation is a green, efficient, alternate technology. Pharmaceuticals are complex molecules. The most efficient way to prepare them is from simply prepared, inexpensive starting molecules with the complexity built in. From our studies, we learned how to develop a new reaction, the desymmetrization of imides by mono hydrogenation. This reaction multiplies the amount of useful molecular complexity that was obtained in a single catalytic step by five. We also construct catalyst-organic frameworks of common catalysts that are presently used once and discarded. Our frameworks are the most reusable chiral catalysts for hydrogenation and cycloisomerizations to date. We aim to prepare continuous flow column reactors with starting material entering the top, and product exiting out the bottom.