SusChEM: Mechanistic Investigations of Oxidative Carbon-Hydrogen Functionalization Reactions

化学部的化学合成计划支持罗德岛大学的Brenton DeBoef教授的项目。德博夫教授正在开发新的化学反应，将碳-氢键转化为碳-氮或碳-碳键。这些反应意义重大，因为大多数有机分子都是由含有碳-碳和碳-氮键的骨架构成的，周围环绕着许多碳-氢键。因此，将选定的碳氢键直接转化为其他键的能力对化学家来说是一个有价值的工具。开发这些新反应的关键是使用新的金和铁基催化剂。这些新反应将帮助化学家构建技术相关的复杂分子，如药物、导电聚合物和有机染料。此外，DeBoef教授还与罗德岛社区学院建立了一个联合研究和培训计划，在该计划中，化学技术专业的学生合成一种潜在的阿尔茨海默氏症药物。这种合作正在通过扩大研究基础设施和科学劳动力培训产生影响。该项目的总体目标是系统地测试关于通过氧化碳-氢(C-H)键激活催化合成碳-碳(C-C)和碳-氮(C-N)键的机理假说。实现这些目标提供了有关贵金属或富含稀土的过渡金属催化剂裂解强的、非酸性的C-H键的机械步骤的基础知识。具体地说，这一建议试图发现金催化的区域选择性C-H胺化反应和铁催化的C-H芳基化反应中的活性催化物种。德博夫曾假设，前一种反应是由一种独特的二聚金物种催化的。一种铁催化剂，其休眠状态是唯一的+1氧化状态，被假设为催化后一反应。通过这项工作获得的基础知识有助于开发新的化学反应和合成方案。德博夫集团为包括妇女和少数族裔在内的研究生和本科生提供了良好的培训环境，为科学领域多元化劳动力的培训做出了贡献。此外，与罗德岛社区学院的外展工作为有抱负的化学技术人员提供了有意义和有市场的研究经验。

The Chemical Synthesis Program of the Chemistry Division supports the project by Professor Brenton DeBoef of the University of Rhode Island. Professor DeBoef is developing new chemical reactions that convert carbon-hydrogen bonds to carbon-nitrogen or carbon-carbon bonds. These reactions are significant because most organic molecules are constructed with a skeletal framework containing carbon-carbon and carbon-nitrogen bonds, surrounded by many carbon-hydrogen bonds on their periphery. Consequently, the ability to directly convert selected carbon-hydrogen bonds to other bonds is a valuable tool for chemists. The key to the development of these new reactions is the use of new gold and iron-based catalysts. These new reactions will help chemists construct technologically relevant, complex molecules such as pharmaceuticals, conducting polymers and organic dyes. Additionally, Professor DeBoef has formed a joint research and training program with the Community College of Rhode Island in which students in the Chemical Technology program synthesize a potential Alzheimer's drug. This collaboration is having an impact by expanding research infrastructure and scientific workforce training. The overarching objective of the project is to systematically test mechanistic hypotheses concerning the catalytic synthesis of carbon-carbon (C-C) and carbon-nitrogen (C-N) bonds via oxidative carbon-hydrogen (C-H) bond activation. Accomplishing these goals provides fundamental knowledge about the mechanistic steps by which noble or earth-abundant transition metal catalysts cleave strong, non-acidic C-H bonds. Specifically, this proposal seeks to discover the active catalytic species in a gold catalyzed regioselective C-H amination reaction and an iron-catalyzed C-H arylation reaction. DeBoef has hypothesized that the former reaction is catalyzed by a unique dimeric gold species. An iron catalyst, whose resting state is in the unique +1 oxidation state, is hypothesized to catalyze the latter reaction. The fundamental knowledge gained by this work facilitates the development of novel chemical reactions and synthetic schemes. The DeBoef group contributes to the training of a diverse workforce in science by providing an excellent training environment for both graduate and undergraduate students, including women and minorities. Additionally, the outreach work with the Community College of Rhode Island provides aspiring chemical technicians with a meaningful and marketable research experience.