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Mimicking sMMOH chemistry: trapping the Sc 3+ -bound nonheme Fe III -O-O-Fe III adduct prior to its conversion into an Fe IV 2(-O)2 core Di-iron systems that activate O2 to form high-valent, oxo-bridged Fe IV 2 or Fe III Fe IV products are of great interest to bio-inorganic chemists due to their relevance to the chemistry of soluble methane mono-oxygenase (sMMOH).In this study, the [Fe III 2(Me3NTB)2(-O)(-O2)] 2+ adduct (Me 3 NTB = tris((1-methyl-1H-benzo[d]imidazol-2-yl)methyl)amine) reacts with two Sc 3+ to break the O-O bond that in turn forms the target Fe IV (-O)2Fe IV product.This study provides the fi rst evidence that a Lewis acid can interact directly with a diferric-peroxo complex to initiate O-O bond cleavage, as evidenced via vibrational and X-ray absorption spectroscopy.