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Title: Homogeneous Catalytic Reduction of O 2 to H 2 O by a Terpyridine-Based FeN 3 O Complex
We report a new terpyridine-based FeN3O catalyst, Fe(tpytbupho)Cl2, which reduces O2 to H2O. Variable concentration and variable temperature spectrochemical studies with decamethylferrocene as a chemical reductant in acetonitrile solution enabled the elucidation of key reaction parameters for the catalytic reduction of O2 to H2O by Fe(tpytbupho)Cl2. These mechanistic studies suggest that a 2 + 2 mechanism is operative, where hydrogen peroxide is produced as a discrete intermediate, prior to further reduction to H2O. Consistent with this proposal, the spectrochemically measured first-order rate constant k (s−1) value for H2O2 reduction is larger than that for O2 reduction. Further, significant H2O2 production is observed under hydrodynamic conditions in rotating ring-disk electrode measurements, where the product can be swept away from the cathode surface before further reduction occurs.
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Award ID(s):
2102156 2018870
Publication Date:
Journal Name:
Inorganic Chemistry
Sponsoring Org:
National Science Foundation
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