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CAS: Catalytic sp3 Carbon-Hydrogen (C-H) Functionalization with Earth Abundant Metals

CAS：利用地球丰富的金属进行催化 sp3 碳-氢 (C-H) 官能化

基本信息

批准号：
2303206
负责人：
Timothy Warren
金额：
$ 49.03万
依托单位：
Michigan State University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2022
资助国家：
美国
起止时间：
2022-12-15 至 2024-10-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=2303206&HistoricalAwards=false
关键词：
CAS Catalytic sp3 Carbon Hydrogen

项目摘要

With this award, the Chemical Catalysis Program of the NSF Division of Chemistry is supporting the research of Professor Timothy Warren of the Department of Chemistry at Georgetown University to develop sustainable catalysts that link abundant chemical building blocks. Using catalysts to link molecular fragments by the formation of new carbon-carbon, carbon-nitrogen, and carbon-oxygen bonds usually requires multi-step chemical processes to first activate the molecular fragments so that they are more reactive. Professor Warren and his team of graduate and undergraduate researchers are designing new ways to connect chemical building blocks using carbon-hydrogen bonds that are difficult to break but found in most feedstock chemicals. The catalysts that are being developed for these reactions are derived from earth abundant copper. These studies involve experiments designed to gain fundamental insight into how the catalysts work to be able to improve their performance in the advanced manufacture of industrial chemicals. This project is providing training for a diverse group of students. Dr. Warren and his group introduce the general public to chemistry at the biannual USA Science and Engineering Festival in Washington, DC. The team will continue to work with young scientists at the beginning of their scientific careers. Each summer a high school student will gain valuable experience and access to a range of more experienced scientists (undergrads, grads, PI) while contributing to the chemical enterprise. Finally, Professor Warren and his students will also provide day-long, hands-on laboratory experiences each summer for rising high school seniors from the Cristo Rey and KIPP networks that serve underprivileged, low-income, and diverse student populations that illustrate connections between Chemistry and the Environment.Catalytic reactions for the conversion of carbon-hydrogen (C-H) bonds in abundant chemical feedstocks to value-added carbon-nitrogen (C-N), carbon-oxygen (C-O), and carbon-carbon (C-C) bonds are valuable for improving the efficiency of synthetic processes. These transformations bypass the steps required to activate reagents and simultaneously decrease waste. Professor Warren and his research group have discovered that a copper-catalyzed radical relay reaction can be used to functionalize C-H bonds and they are currently investigating new synthetic transformations that can be achieved with this catalytic system. These studies involve optimizing the catalyst to accommodate new types of reagents to react with the C-H bonds, exploring new oxidants to decrease the excess amount of alkane currently required, and investigating asymmetric systems for C-H amidation. In addition, fundamental mechanistic studies are being performed to collect information that will facilitate further development and optimization. These research activities also serve as a training ground for a diverse group of graduate, undergraduate, and high school students.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

有了这个奖项，NSF化学部的化学催化计划正在支持乔治敦大学化学系的Timothy Warren教授的研究，以开发可持续的催化剂，将丰富的化学构件连接起来。使用催化剂通过形成新的碳-碳、碳-氮和碳-氧键来连接分子片段通常需要多步化学过程来首先活化分子片段，使得它们更具反应性。沃伦教授和他的研究生和本科生研究人员团队正在设计新的方法，使用难以打破但在大多数原料化学品中发现的碳氢键连接化学构件。为这些反应开发的催化剂来自地球上丰富的铜。这些研究涉及旨在深入了解催化剂如何工作的实验，以便能够提高其在工业化学品先进制造中的性能。该项目为不同的学生群体提供培训。沃伦博士和他的小组在华盛顿举行的两年一度的美国科学与工程节上向公众介绍化学。该团队将继续与年轻科学家在他们的科学生涯开始时合作。每年夏天，一名高中生将获得宝贵的经验，并接触到一系列更有经验的科学家（本科生，研究生，PI），同时为化工企业做出贡献。最后，沃伦教授和他的学生还将提供为期一天的，动手实验室的经验，每年夏天上升的高中高年级学生从克里斯托雷伊和KIPP网络，服务于贫困，低收入，和不同的学生群体，说明化学与环境之间的联系。催化反应，将丰富的化学原料中的碳氢（C-H）键转化为增值的碳氮（C-N）N）、碳-氧（C-O）和碳-碳（C-C）键对于提高合成工艺的效率是有价值的。这些转化绕过了激活试剂所需的步骤，同时减少了浪费。Warren教授和他的研究小组发现，铜催化的自由基中继反应可用于官能化C-H键，他们目前正在研究可以用这种催化体系实现的新的合成转化。这些研究涉及优化催化剂以适应新型试剂与C-H键反应，探索新的氧化剂以减少目前所需的过量烷烃，并研究C-H酰胺化的不对称体系。此外，正在进行基本的机理研究，以收集有助于进一步开发和优化的信息。这些研究活动也是研究生、本科生和高中生的培训基地。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。