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

在化学系化学催化项目的支持下，马奎特大学的Chae Yi教授正在研究使用环境可持续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的新方法。该方法依赖于使用过渡金属介导的催化中的新兴概念，该概念允许分子框架在传统上抵抗操纵的键处被破坏和重组。这些研究将可能导致催化键活化领域的根本性进展，预计所获得的知识将导致在制备制药和其他有价值产品所需的复杂有机分子方面的经济和环境改进。资助项目的更广泛影响将扩展到支持暑期实习，这将使当地大学STEM（科学，技术，工程和数学）项目的本科生能够在彝族实验室获得研究经验。此外，该奖项将使易教授能够在当地的高中和大学从事外展工作，这将有助于促进具有不同背景的学生在科学和工程方面的职业生涯，其中许多人属于目前STEM劳动力中代表性不足的群体。该资助项目将侧重于开发基于碳-碳和碳-氮键活化（断裂）的有机合成新催化方法。将研究由具有氧化还原活性邻苯二酚配体的定义明确的钌催化剂介导的此类过程的范围和机理方面，并探索其用于重整生物质衍生的有机商品的合成应用。在这些研究过程中，易实验室将奋进于开发一系列多功能，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。

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.