Design of Lewis-Acid Appended Catalysts for Cooperative Activation

Regents Of The University Of Michigan - Ann Arbor, Ann Arbor MI

Investigators

Abstract

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.