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

Dian Wang; Florian Loose; Paul J. Chirik; Robert R. Knowles

doi:10.1021/jacs.8b12957

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

Dian Wang, Florian Loose, Paul J. Chirik, Robert R. Knowles

Research output: Contribution to journal › Article › peer-review

42 Scopus citations

Abstract

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 )Mn ^V N 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 Brønsted 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.

Original language	English (US)
Pages (from-to)	4795-4799
Number of pages	5
Journal	Journal of the American Chemical Society
Volume	141
Issue number	12
DOIs	https://doi.org/10.1021/jacs.8b12957
State	Published - Mar 27 2019

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.8b12957

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

abstract = " 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 )Mn V N 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 Br{\o}nsted 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. ",

author = "Dian Wang and Florian Loose and Chirik, {Paul J.} and Knowles, {Robert R.}",

note = "Funding Information: Financial support was provided by the Andlinger Center for Energy and the Environment (Princeton University). F.L. acknowledges support by DFG Research Fellowship (LO 2377/1-1). P.J.C. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Science (DE-SC0006498). Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

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doi = "10.1021/jacs.8b12957",

language = "English (US)",

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AU - Wang, Dian

AU - Loose, Florian

AU - Chirik, Paul J.

AU - Knowles, Robert R.

N1 - Funding Information: Financial support was provided by the Andlinger Center for Energy and the Environment (Princeton University). F.L. acknowledges support by DFG Research Fellowship (LO 2377/1-1). P.J.C. acknowledges support from the U.S. Department of Energy, Office of Science, Basic Energy Science (DE-SC0006498). Publisher Copyright: © 2019 American Chemical Society.

PY - 2019/3/27

Y1 - 2019/3/27

N2 - 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 )Mn V N 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 Brønsted 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.

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

Abstract

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