CAREER: Design of Catalysts for Cooperative Small Molecule Activation

在这个由化学系化学催化项目资助的项目中，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激活和功能化反应的过渡金属配合物。这项工作旨在为小分子（如H2）如何在金属配合物的二级配位球中的刘易斯酸和碱位点的帮助下被激活提供基本的见解。该研究的目标是基于钳的金属配体支架，其特征是悬垂的硼烷和胺位点。这些将被选择来赋予一个高度极化的二级配位球环境，这将使系统偏向于异裂键激活/转移反应。定向递送H-E （E=H, SiR3, BR2）是一个目标。该教育计划涉及开发一种真实的研究设计方法来教授本科实验课程。假设驱动实验，模拟真实世界的研究环境，将被纳入低水平和高水平的本科实验课程。这应该能让学生更好地为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量化学转化策略带来的潜在社会效益。这些可能最终适用于地球上丰富的金属。氢化反应是应用最广泛的催化反应之一，涉及许多工业部门，包括石油化工、食品和制药生产。该项目侧重于开发含有多个反应位点的过渡金属化合物，以促进化学原料的氢化反应。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定的化学反应，产生最小的废物，并且含有丰富的金属。教育部分将为本科生和研究生提供跨学科的培训，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.