Many enzymes utilize polynuclear metal cofactors to catalyze a variety of small molecule activation reactions critical for life. In order to design better functional mimics and analogs, we must first understand the electronic structure that facilitates reactivity. Using polynucleating ligands, we have synthesized a variety of open-shell clusters with trinuclear cores that we can characterize with high fidelity. Using these clusters, we sought to answer the following questions: (1) how do weak-field clusters mediate redox chemistry; (2) how can the electronic structure of said clusters be altered by secondary coordination elements (H, K, Au); and (3) can we use clusters as multi-electron reservoirs as ancillary ligands to transition metals. In pursuit of these goals, we have isolated a variety of µ3-nitride and µ3-imido triiron complexes and investigated the electronic structure of the complexes through 57Fe Mössbauer spectroscopy, cyclic voltammetry and SQUID magnetometry. By varying the secondary coordination environment of the µ3-nitrogen, we are able to investigate how perturbations to the local coordination environment effect differences in electronic structure. We are investigating the ability of the µ3-nitride and µ3-imido complexes to serve as bulky anionic ligands for low coordinate metal centers.

Investigating multi-electron structure and reactivity with trinuclear µ3-nitride complexes

255th National Meeting (2018)

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