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- W2945476616 abstract "Catalysts for the oxidation of NH3 are critical for the utilization of NH3 as a large-scale energy carrier. Molecular catalysts capable of oxidizing NH3 to N2 are rare. This report describes the use of [Cp*Ru(PtBu2NPh2)(15NH3)][BArF4], (PtBu2NPh2=1,5-di(phenylaza)-3,7-di(tert-butylphospha)cyclooctane; ArF=3,5-(CF3)2C6H3), to catalytically oxidize NH3 to dinitrogen under ambient conditions. The cleavage of six N−H bonds and the formation of an N≡N bond was achieved by coupling H+ and e− transfers as net hydrogen atom abstraction (HAA) steps using the 2,4,6-tri-tert-butylphenoxyl radical (tBu3ArO.) as the H atom acceptor. Employing an excess of tBu3ArO. under 1 atm of NH3 gas at 23 °C resulted in up to ten turnovers. Nitrogen isotopic (15N) labeling studies provide initial mechanistic information suggesting a monometallic pathway during the N⋅⋅⋅N bond-forming step in the catalytic cycle." @default.
- W2945476616 created "2019-05-29" @default.
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- W2945476616 date "2019-06-11" @default.
- W2945476616 modified "2023-10-11" @default.
- W2945476616 title "Catalytic Ammonia Oxidation to Dinitrogen by Hydrogen Atom Abstraction" @default.
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- W2945476616 doi "https://doi.org/10.1002/anie.201903221" @default.
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