Development of Catalytic Coupling Methods via Unreactive C-C and C-N Bond Activation

在化学系化学催化计划的支持下，马奎特大学的蔡毅教授正在研究新的方法，利用环境可持续的催化过程将石油和生物质衍生的商品化学品升级为增值材料。这种方法依赖于过渡金属介导的催化中新兴概念的使用，这些概念允许在传统上抵制操纵的键上打破和改革分子框架。这些研究可能会导致催化键活化领域的根本性进展，所获得的知识预计将导致制备复杂有机分子的经济和环境改善，这些复杂有机分子是制造药物和其他有价值的产品所需的。该资助项目的更广泛影响将延伸到支持暑期实习，允许当地大学STEM(科学、技术、工程和数学)专业的本科生在YI实验室获得研究经验。此外，该奖项将使易教授能够参与当地高中和大学的外联工作，这将有助于促进不同背景的学生在科学和工程领域的职业生涯，其中许多学生属于目前STEM劳动力中代表性较低的群体。资助的项目将侧重于开发基于碳-碳键和碳-氮键的活化(断裂)的有机合成新催化方法。本课程将研究以氧化还原活性邻苯二酚为配体的定义明确的Ru催化剂所介导的这类过程的范围和机理，并探索其在生物质衍生有机产品重整中的合成应用。在这些研究过程中，YI实验室将努力开发一系列多组分脱氨基催化偶联方法，将羰基化合物与烯胺融合为一种有效的策略，用于阐述各种与产生药物活性物质相关的杂环系统。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

With the support of the Chemical Catalysis Program in the Division of Chemistry, Professor Chae Yi of Marquette University is studying new methods to upgrade petroleum and biomass-derived commodity chemicals into value-added materials using environmentally sustainable catalytic processes. The approach relies on the use of emerging concepts in transition-metal mediated catalysis that allow for molecular frameworks to be broken and reformed at bonds that have traditionally resisted manipulation. The studies will likely lead to fundamental advances in the field of catalytic bond activation and the knowledge gained is anticipated to lead to economic and environmental improvements in the preparation of complex organic molecules needed for the manufacture of pharmaceuticals and other valuable products. The broader impacts of the funded project shall extend to supporting summer internships that will allow for undergraduate students from local college STEM (science, technology, engineering and mathematics) programs to receive research experiences in the Yi laboratory. In addition, the award will enable Professor Yi to engage in outreach efforts at local high schools and colleges that will serve to promote careers in science and engineering for students with diverse backgrounds and many of whom belonging to groups underrepresented in the current STEM workforce. The funded project will focus on the development of new catalytic methods for organic synthesis based on the activation (rupture) of carbon-carbon and carbon-nitrogen bonds. The scope and mechanistic aspects of such processes as mediated by well-defined ruthenium catalysts with redox-active catechol ligands will be investigated and their synthetic applications for reforming biomass-derived organic commodities will be explored. During the course of these studies, the Yi laboratory will endeavor to develop a series of multi-component deaminative catalytic coupling methods that fuse carbonyl compounds with enamines as an efficient strategy for the elaboration of a variety of heterocyclic systems of relevance for the generation of pharmaceutically active substances.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.