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). Contrastingly, few synthetic clusters can effect such reactions under similarly mild conditions. To understand the structural and electronic parameters that dictate cooperative effects in metal clusters, we employ macrobicycles as ligands to enforce a priori control of the electronic environment and the spatial arrangement of metal ions within multimetalic compounds. Recent results from our ongoing work on small molecule activation by these template multimetallic compounds include N2 fixation and CO2 reduction. These results are a departure from the reactivity of the monometallic analogs, providing a framework for describing the design criteria for effectively harnessing cooperative effects in bond activation.

Engineering multimetallic compounds to activate small molecules

2019 Spring National Meeting

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