Abstract: 

In nature, metalloenzymes have evolved to perform important chemical reactions by precisely controlling both the primary and secondary coordination spheres of their metallocofactors. This dissertation outlines research on developing new bio-inspired metal complexes to replicate the local environments and functional aspects of metalloenzyme active sites. These synthetic analogues are supported by rigid tripodal ligand frameworks with appended functional groups that are positioned proximal to a metal ion to promote intramolecular H-bond interactions. These ligand scaffolds can be systematically modified to examine the impact of these interactions on the chemistry of monomeric metal species. Additionally, this work includes the preparation of bimetallic complexes to explore proton-mediated spin state transitions and the potential influence of magnetic coupling between metal centers in regulating their thermodynamic properties. The results of this dissertation aim to provide insights into the structure-function relationships of coordination complexes and guide the design of bimetallic systems with tunable magnetic properties.