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，最大限度地提高催化剂的反应性、寿命和可重复使用性，并利用这些信息来指导制备更好的催化剂和反应。我们制备了活性溶解催化剂，高度可重复使用的固体聚合物催化剂框架，以及定制的纳米颗粒。野依酮加氢反应中重要的、应用广泛的中间体我们已经完成了大部分中间体的制备和研究。从这项研究中，我们学会了如何开发一个系统，在非常温和的条件下氢化酯来制造酒精。目前，从酯类到醇类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、高效的替代技术。药物是复杂的分子。制备它们最有效的方法是从简单的、廉价的、具有复杂性的初始分子开始。从我们的研究中，我们学会了如何开发一个新的反应，亚胺的单氢脱对称。这个反应使在单一催化步骤中获得的有用分子复杂性增加了五倍。我们还构建了目前使用一次并丢弃的常见催化剂的催化剂有机框架。我们的框架是迄今为止最可重复使用的氢化和环异构化手性催化剂。我们的目标是制备连续流塔式反应器，起始物料从顶部进入，产物从底部流出。

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.