In this CAREER project, Professor Yuyang Dong of the Department of Chemistry at Colorado State University is developing a series of square-planar base-metal complexes to understand how their electronic structures control catalytic performance. The goal of this research is to use these structure-reactivity relationships to guide the development of base-metal catalytic processes to reduce the reliance on rare and costly precious metals. By establishing these design principles, the project could lead to the next-generation catalysts for the advanced manufacturing of pharmaceuticals, agrochemicals, and novel materials. The project lies at the interface of synthetic organic chemistry, inorganic chemistry, and catalysis, making it well-suited to provide high-level education and training for scientists at multiple career stages. Integrated educational activities will engage local high school students, expand access to advanced inorganic chemistry education through community-college partnerships, and share research-inspired learning modules to make the problem-solving process behind modern synthetic chemistry more accessible to a broader audience. This project could establish electronic structure-reactivity relationships across a series of high-spin catalytic intermediates. The central advance is the use of weak-field pincer ligands to stabilize and characterize highly reactive open-shell species that are typically too short-lived to observe. These include metal-ligand multiply bonded complexes involved in group-transfer catalysis, open-shell metal-boryl compounds relevant to radical borylation, and high-spin metal-alkyl intermediates proposed in olefin functionalization. By isolating these complexes and correlating their spin states, frontier orbitals, redox properties, and ligand-field environments with stoichiometric and catalytic reactivity, this project could define the core principles to control challenging single-electron processes. These insights are expected to