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The new complex [Mn(bipyalk)(H2O)(μ-O)2Mn(bipyalk)](OTf)2 (bipyalk = 2-([2,2'-bipyridin]-6-yl)propan-2-ate) catalyzes oxygen evolution with a TOF of 0.0055 s when driven by the sacrificial oxidant KHSO5 in water. It is proposed on the… Click to show full abstract
The new complex [Mn(bipyalk)(H2O)(μ-O)2Mn(bipyalk)](OTf)2 (bipyalk = 2-([2,2'-bipyridin]-6-yl)propan-2-ate) catalyzes oxygen evolution with a TOF of 0.0055 s when driven by the sacrificial oxidant KHSO5 in water. It is proposed on the basis of EPR experiments that the catalyst proceeds through a Mn(μ-O)2Mn =O intermediate supported by the highly donating tertiary alkoxide moiety of the ligand. The Mn(IV,IV) dimer can also be formed electrochemically from its precursor, Mn(bipyalkH)Cl2. A related series of bis-ligated monomers of the type [Mn (bipyalkHx)(bipyalkHy)](PF6)2 is also reported, where the dication features Mn, Mn, and Mn oxidation states and corresponding protonation states. Electrochemical data on this series underscore the importance of proton loss at the alcohol/alkoxide moiety during oxidation to maintain low overpotentials required for catalysis.
Journal Title: European Journal of Inorganic Chemistry
Year Published: 2019
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