4.8 Article

N-H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 12, 页码 4795-4799

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b12957

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资金

  1. Andlinger Center for Energy and the Environment (Princeton University)
  2. DFG Research Fellowship [LO 2377/1-1]
  3. U.S. Department of Energy, Office of Science, Basic Energy Science [DE-SC0006498]

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A method for the reduction of a manganese nitride to ammonia is reported, where light driven proton-coupled electron transfer enables the formation of weak N-H bonds. Photoreduction of (sal(tBu))(MnN)-N-V to ammonia and a Mn(II) complex has been accomplished using 9,10-dihydroacridine and a combination of an appropriately matched photoredox catalyst and weak Bronsted acid. Acid-reductant pairs with effective bond dissociation free energies between 35 and 46 kcal/mol exhibited high efficiencies. This light-driven method may provide a blueprint for new approaches to catalytic homogeneous ammonia synthesis under ambient conditions.

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