CAREER: Design of Catalysts for Cooperative Small Molecule Activation

在这个由化学部化学催化计划资助的项目中，密歇根大学的Nathaniel Szymczak教授将开发能够与金属配位底物进行键活化和功能化反应的过渡金属络合物。这项工作旨在提供基本的见解，如何小分子，如H2，可以激活的协助下，从刘易斯酸和碱的网站在二级配位领域的金属络合物。这项研究的目标钳为基础的金属配体支架，功能悬垂硼烷和胺网站。这些将被选择以赋予高度极化的次级配位球环境，其将使系统偏向异裂键活化/转移反应。H-E（E=H，SiR 3，BR 2）的定向递送是一个目标。该教育计划涉及一个真实的研究设计方法来教学本科实验室课程的发展。假设驱动的实验，模拟现实世界的研究环境，将被纳入较低和较高水平的本科实验室课程。这应该更好地为学生在STEM领域的职业生涯做好准备。这项工作的更广泛影响包括发现低能耗化学转化策略带来的潜在社会效益。它们最终可能会适应地球上丰富的金属。氢化反应是最广泛使用的催化反应之一，涵盖许多工业部门，包括石油化工，食品和制药生产。该项目的重点是开发含有多个反应位点的过渡金属化合物，以促进化学原料的加氢反应。通过使用具有高度模块化单元的系统，合成催化剂的目标是最终可扩展，促进适用于许多领域的高度特异性化学反应，产生最少的废物，并含有地球丰富的金属。教育部分将为本科生和研究生提供跨学科培训，为他们在教学，工业化学，国家实验室或公共政策方面的职业生涯做好准备。

In this project funded by the Chemical Catalysis program of the Chemistry Division, Professor Nathaniel Szymczak of The University of Michigan will develop transition metal complexes capable of cooperative interactions with metal-coordinated substrates for bond activation and functionalization reactions. The work seeks to provide fundamental insights into how small molecules, such as H2, can be activated with assistance from Lewis acid and base sites in the secondary coordination sphere of a metal complex. The study targets pincer-based metal-ligand scaffolds that feature pendent borane and amine sites. These will be selected to confer a highly polarized secondary coordination sphere environment that will bias the system toward heterolytic bond activation/transfer reactions. The directed delivery of H-E (E=H, SiR3, BR2) is a goal. The Educational Plan involves the development of an authentic research design approach to teaching undergraduate lab courses. Hypothesis-driven experimentation, which simulates a real-world research environment, will be incorporated into both lower and upper level undergraduate laboratory courses. This should better prepare students for careers in STEM fields. The broader impacts of this work include potential societal benefits from the discovery of low-energy chemical conversion strategies. These may ultimately be adapted to earth-abundant metals. Hydrogenation reactions are among the widest used catalytic reactions, encompassing many industrial sectors, including petrochemical, food, and pharmaceutical production. This project focuses on the development of transition metal compounds that contain multiple reactive sites in order to promote otherwise difficult hydrogenation reactions of chemical feedstocks. By using a system with highly modular units, synthetic catalysts are targeted that are ultimately scalable, promote highly specific chemical reactions applicable to many fields, generate minimal waste, and contain earth-abundant metals. The educational component will provide interdisciplinary training for undergraduate and graduate students to prepare them for careers in teaching, in industrial chemistry, at a national lab, or in public policy.