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Title: Cyclophane-Supported Trimetallic Clusters: N2 cleavage, O2 activation and O-atom transfer reactivity
Biological systems utilize metal-ion redox cooperativity within metal clusters to catalyze multi-electron redox reactions under ambient conditions and at biologically-accessible reduction potentials (e.g., N2 reduction). These reactions are essential to atom cycles in biosphere and are also of great societal value for green energy and improved food production. In contrast, few synthetic clusters are capable of performing these reactions, suggesting that the protein matrix affords unique control of electronic and steric effects to access this reactivity. In an attempt to understand how structural and electronic parameters dictate cooperative effects in metal clusters, we employ macrobicycles as ligands to enforce a priori control of the electronic environment and the relative spatial arrangement of metal ions within trimetallic clusters. Results of our ongoing work including dinitrogen coordination and reduction, the reactivity of bridging hydrides, and dioxygen activation will be presented.