Multinuclear metal ensembles, and their attendant reactivity, are an essential feature of biotic metabolism where they serve both as electron transfer agents and molecular catalysts. We believe that both these modes of reactivity are enabled by the high spin states that are common to such clusters, as well as by the redox buffering that may occur when an electron transfer event is spread across multiple metal centers. Therefore, in an effort to obtain a synthetic system that will facilitate both electron transfer and small molecule transformation events, we have designed a hexanuclear iron cluster supported solely by bridging amide donors. This cluster is high spin (S = 6) and displays ready access to a wide range of oxidation states at mild potentials. Each of the cluster’s redox events is delocalized across all six metal centers in a manner that reflects the redox buffering we had sought to achieve with these clusters. Our efforts exploring the small molecule reactivity of highly solubilized derivatives of these clusters will be discussed.

Rational design: Programming small molecule reactivity in a multinuclear iron cluster

250th National Meeting (2015)

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