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 (saltBu)MnVN 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 35–46 kcal/mol exhibited high efficiencies. As a result, this light-driven method may provide a blueprint for new approaches to catalytic homogenous ammonia synthesis under ambient conditions.
- Publication Date:
- Research Org.:
- Princeton Univ., NJ (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1506845
- Grant/Contract Number:
- SC0006498
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 141; Journal Issue: 12; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Wang, Dian, Loose, Florian, Chirik, Paul J., and Knowles, Robert R. N–H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer. United States: N. p., 2019.
Web. doi:10.1021/jacs.8b12957.
Wang, Dian, Loose, Florian, Chirik, Paul J., & Knowles, Robert R. N–H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer. United States. https://doi.org/10.1021/jacs.8b12957
Wang, Dian, Loose, Florian, Chirik, Paul J., and Knowles, Robert R. Mon .
"N–H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer". United States. https://doi.org/10.1021/jacs.8b12957. https://www.osti.gov/servlets/purl/1506845.
@article{osti_1506845,
title = {N–H Bond Formation in a Manganese(V) Nitride Yields Ammonia by Light-Driven Proton-Coupled Electron Transfer},
author = {Wang, Dian and Loose, Florian and Chirik, Paul J. and Knowles, Robert R.},
abstractNote = {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 (saltBu)MnVN 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 35–46 kcal/mol exhibited high efficiencies. As a result, this light-driven method may provide a blueprint for new approaches to catalytic homogenous ammonia synthesis under ambient conditions.},
doi = {10.1021/jacs.8b12957},
journal = {Journal of the American Chemical Society},
number = 12,
volume = 141,
place = {United States},
year = {Mon Feb 25 00:00:00 EST 2019},
month = {Mon Feb 25 00:00:00 EST 2019}
}
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