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.

通过此奖项，NSF化学部的化学催化计划支持乔治敦大学化学系教授的蒂莫西·沃伦（Timothy Warren）的研究，以开发可持续的催化剂，这些催化剂将丰富的化学构建块联系起来。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才能首先激活分子片段，以使它们更具反应性。沃伦（Warren）教授及其毕业生和本科研究人员的团队正在设计新的方法来使用碳氢键连接化学构建块，这些碳纤维键很难破裂，但在大多数原料化学物质中都可以找到。为这些反应开发的催化剂来自地球丰富的铜。这些研究涉及旨在获得有关催化剂如何工作以提高其在工业化学品高级生产中的性能的基本见解的实验。该项目正在为各种学生提供培训。沃伦（Warren）博士和他的小组在华盛顿特区的两年一年度美国科学与工程节上向公众介绍化学。该团队将在科学职业开始时继续与年轻科学家合作。每年夏天，一名高中生将获得宝贵的经验，并获得一系列经验丰富的科学家（本科生，毕业生，PI），同时为化学企业做出贡献。最后，沃伦教授和他的学生还将在每年夏天提供一整天的动手实验室经验，以供升高的高中生和克里斯托·雷伊（Cristo Rey）和基普网络（Kipp Networks）提供服务，这些网络服务于贫困，低收入和多样化的学生人群，以说明化学与环境之间的联系。碳氮（C-N），碳氧（C-O）和碳碳（C-C）键对于提高合成过程的效率很有价值。这些转换绕过激活试剂并同时减少废物所需的步骤。沃伦（Warren）教授及其研究小组发现，铜催化的激进继电器反应可用于使C-H键官能化，他们目前正在研究该催化系统可以实现的新合成转化。这些研究涉及优化催化剂，以适应新型的试剂与C-H键反应，探索新的氧化剂以减少当前所需的烷烃过量量，并研究C-H胺的不对称系统。此外，正在进行基本的机械研究以收集将有助于进一步发展和优化的信息。这些研究活动还为多样化的研究生，本科和高中生的培训理由。该奖项反映了NSF的法定任务，并被认为是值得通过基金会的知识分子优点和更广泛的影响评估标准通过评估来获得支持的。