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Soluble methane monooxygenase (sMMO) carries out methane oxidation at 4 °C and under ambient pressure in a catalytic cycle involving the formation of a peroxodiiron(III) intermediate ( P ) from the oxygenation of the diiron(II) enzyme and its subsequent conversion to Q , the diiron(IV) oxidant that hydroxylates methane. Synthetic diiron(IV) complexes that can serve as models for Q are rare and have not been generated by a reaction sequence analogous to that of sMMO. In this work, we show that [Fe II (Me 3 NTB)(CH 3 CN)](CF 3 SO 3 ) 2 (Me 3 NTB = tris((1-methyl-1 H -benzo[d]imidazol-2-yl)methyl)amine) ( 1 ) reacts with O 2 in the presence of base, generating a (μ-1,2-peroxo)diiron(III) adduct with a low O-O stretching frequency of 825 cm -1 and a short Fe···Fe distance of 3.07 Å. Even more interesting is the observation that the peroxodiiron(III) complex undergoes O-O bond cleavage upon treatment with the Lewis acid Sc 3+ and transforms into a bis(μ-oxo)diiron(IV) complex, thus providing a synthetic precedent for the analogous conversion of P to Q in the catalytic cycle of sMMO.

journal of the american chemical society

Sc3+-Promoted O–O Bond Cleavage of a (μ-1,2-Peroxo)diiron(III) Species Formed from an Iron(II) Precursor and O2 to Generate a Complex with an FeIV2(μ-O)2 Core