Design of Lewis-Acid Appended Catalysts for Cooperative Activation

在化学系化学催化项目的支持下，密歇根大学的Nathaniel Szymczak教授将研究构建多功能催化剂的新策略，这些催化剂具有与碳建立/断开键的潜力，这是有机合成的核心目标，涵盖许多工业部门，包括石化、材料开发和制药生产。在这个项目中，Szymczak和他的团队正在开发一种分子工具包，以制备包含多个反应位点的过渡金属化合物。这些催化剂将在将容易获得的化学前体转化为增值产品的背景下进行研究，目前的方法有别于传统方法，具有潜在的优势。这一方法旨在通过合理的设计原则，促进开发可持续化学生产所需的分子催化剂所需的基础科学。这项工作的更广泛影响包括发现低能量化学转化战略以制造燃料、平台化学品和复杂的药剂所带来的社会效益。此外，参与该项目的本科生和研究生将接受跨学科的科学培训，为他们从事最先进的科学研究做好准备。Szymczak教授正在开发一个跨越多个机构级别的全国性会议系列，让学生参与到科学研究和数据解释的各个方面。为了进一步提高年轻学生的科学素养，他和他在密歇根的研究生和本科生在当地许多活动和学校与学生接触。在这个项目中，Nathaniel Szymczak教授和他在密歇根大学的研究团队将研究合成策略，以制备能够与金属配位的底物多点结合的新的过渡金属络合物，最终将用于控制底物的活化和功能化反应。这种方法不同于用于制备均相催化剂的典型策略，它侧重于将多个Lewis酸碱相互作用作为主要设计工具。该项目旨在确定可广泛用于制备具有可变距离和酸度的附加Lewis酸性基团的配体支架的合成原理。这些努力可以使人们能够获得配体平台，其中刘易斯酸性单元在一系列初级球体上保持不变，从而导致以前无法获得的化合物。设计工作的目的是为路易斯酸辅助的C-C和C-X化学键的结合、活化和功能化提供结构/功能指南，包括有机腈官能化的区域化学控制：挑战C-C键(去)结构反应。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 Nathaniel Szymczak of the University of Michigan will study new strategies to construct multifunctional catalysts that have the potential to make/break bonds to carbon, a central goal of organic synthesis, encompassing many industrial sectors, including petrochemical, materials development, and pharmaceutical production. In this project, Szymczak and his team are developing a molecular toolkit to prepare transition metal compounds that contain multiple reactive sites. These catalysts will be studied within the context of converting readily accessible chemical precursors into value-added products, with the current approach being distinct from conventional methods and potentially advantageous. This approach aims to advance the basic science needed to develop molecular catalysts for sustainable chemical production through rational design principles. The broader impacts of this work include societal benefits from the discovery of low-energy chemical conversion strategies to make fuels, platform chemicals, and complex pharmaceutical agents. In addition, undergraduate and graduate students working on this project will receive interdisciplinary scientific training to prepare them for careers in state-of-the-art science research. Professor Szymczak is developing a nationwide meeting series across multiple institutional levels to engage students in aspects of scientific research and data interpretation. To further improve scientific literacy among younger students, he and his graduate and undergraduate students at Michigan are engaging with students at numerous local events and schools.In this project, Professor Nathaniel Szymczak and his research team at the University of Michigan will study synthetic strategies to prepare new transition metal complexes capable of multi-point binding to metal-coordinated substrates, which will ultimately be used to control substrate activation and functionalization reactions. This approach diverges from typical strategies used to prepare homogeneous catalysts, by focusing on multiple Lewis acid/base interactions as a primary design tool. This project aims to identify synthetic principles that can be broadly used to prepare ligand scaffolds containing appended Lewis acidic groups at variable distance and acidity. These efforts could enable access to ligand platforms wherein a Lewis acidic unit is maintained across a wide set of primary sphere donors, leading to compounds that have been previously inaccessible. The design efforts are being pursued to provide structure/function guidelines into Lewis-acid assisted binding, activation, and functionalization of C-C and C-X chemical bonds, including regiochemical control of organonitrile functionalization: challenging C-C bond (de)construction reactions.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.