Polynuclear metalloenzymes are at the core of important biological transformations such as nitrogen fixation and water oxidation.  With nature as our inspiration, we sought to rationally design a series of polynuclear complexes in which the metal centers are in close proximity.  A series of trinuclear, (LNH)2M3 (where LNH = MeC(CH2NHPh-o-NH2)3 and M= Mn or Co),  and hexanuclear, (LNH)2M6 complexes have been synthesized.  Varying the substituents on the ligand periphery, results in perturbations to the electronic structure of the resultant molecules.  Group transfer reactions to the trinuclear metal complexes as well as the synthesis of a novel Co3(�3-N) will be discussed.  Oxidation of the trinuclear manganese clusters has thus far been achieved via group transfer reagents, resulting in site-isolated oxidation and formation of hexanuclear manganese complexes.  These compounds are quite novel in that they contain an interstitial �6-O or �6-N at the center of an octahedron of manganese metals.

Driving polynuclear reaction chemistry

243rd National Meeting (2012)

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