We report the oxidation of alkane and alkene substrates catalyzed by first-row transition metal complexes with the hexadentate ligand N,N'-bis(2-pyridylmethyl)-bis(ethylacetate)-1,2-ethanediamine (debpn). The Mn(II) and Fe(II) debpn complexes contain heptacoordinate metal centers. As catalysts, these compounds are less active than hexacoordinate analogs prepared from electronically similar tetradentate ligands. Less sterically congested substrates react more readily, suggesting that part of the decreased activity results from increased steric repulsions between the ligand and the substrate. Computational analysis suggests that the divalent oxidation states of the metal compounds are stabilized by the additional donor atom; this would further increase the free energy barrier for reactivity if similar oxidants are operable in the reactive pathways.

Hydrocarbon oxidation catalyzed by heptacoordinate Mn(II) and Fe(II) complexes

244th National Meeting (2012)

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