Innovative Tools for Chemical Synthesis: Cyclase-Inspired Catalysis, Shuttle Catalysis, and Tandem Catalysis

项目摘要（来自MIRA原始奖项GM 127071） 这项研究计划的重点是解决化学结构和反应性的差距，通过 催化的力量受到金属酶的启发，我的实验室设计，研究， 用于化学合成的创新工具，克服了对手性助剂的需求， 化学计量活化剂。所提出的交叉耦合方法的特点是使用 常见的官能团（例如，醛、胺、炔和烯烃）并产生新的 碳-碳和碳-氮键，具有优异的原子经济性。广泛的手性 图案可以通过这种方法访问，所获得的见解将最终提高我们的 控制化学反应和构建化学结构的能力。反过来，这种知识大大 增强了我们发现治疗人类疾病的新药的能力， 大规模使用这些药物。该计划具有许多新的方向， 令人信服的初步数据，包括环化酶启发的催化，穿梭催化，和串联 催化作用除了实用价值，该计划将提供基本的见解使用 各种催化剂，包括铑、钌、钴和镍，用于活化， 碳-氢键的功能化--现代有机化学中一个长期存在的挑战 化学

Project Summary (from the original MIRA award GM127071) This research program focuses on addressing gaps in chemical structure and reactivity through the power of catalysis. Inspired by metalloenzymes, my laboratory designs, studies, and invents innovative tools for chemical synthesis that overcome the need for chiral auxiliaries and stoichiometric activating agents. The cross-coupling methods proposed feature the use of common functional groups (e.g., aldehydes, amines, alkynes, and alkenes) and generate new carbon-carbon and carbon-nitrogen bond with excellent atom economy. A wide range of chiral motifs can be accessed by this approach and the insights gained will ultimately enhance our ability to control chemical reactivity and build chemical structures. In turn, this knowledge greatly augments our ability to discover new medicines for treating human diseases, as well as prepare these medicines on large scale. The program features many new directions supported by compelling preliminary data including cyclase-inspired catalysis, shuttle catalysis, and tandem catalysis. Besides the practical value, this program will provide fundamental insights into the use of various catalysts, including rhodium, ruthenium, cobalt, and nickel, for the activation and functionalization of carbon-hydrogen bonds—a long standing challenge in modern organic chemistry