Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes
Abstract
Nitrogen fixation, the six-electron/six-proton reduction of N2, to give NH3, is one of the most challenging and important chemical transformations. Notwithstanding the barriers associated with this reaction, significant progress has been made in developing molecular complexes that reduce N2 into its bioavailable form, NH3. This progress is driven by the dual aims of better understanding biological nitrogenases and improving upon industrial nitrogen fixation. In this review, we highlight both mechanistic understanding of nitrogen fixation that has been developed, as well as advances in yields, efficiencies, and rates that make molecular alternatives to nitrogen fixation increasingly appealing. We begin with a historical discussion of N2 functionalization chemistry that traverses a timeline of events leading up to the discovery of the first bona fide molecular catalyst system and follow with a comprehensive overview of d-block compounds that have been targeted as catalysts up to and including 2019. Furthermore, we end with a summary of lessons learned from this significant research effort and last offer a discussion of key remaining challenges in the field.
- Authors:
-
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Publication Date:
- Research Org.:
- California Institute of Technology (CalTech), Pasadena, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1698026
- Grant/Contract Number:
- SC0019136
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Reviews
- Additional Journal Information:
- Journal Volume: 120; Journal Issue: 12; Journal ID: ISSN 0009-2665
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Reaction mechanisms; Ligands; Ammonia; Catalysts; Nitrogen
Citation Formats
Chalkley, Matthew J., Drover, Marcus W., and Peters, Jonas C. Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes. United States: N. p., 2020.
Web. doi:10.1021/acs.chemrev.9b00638.
Chalkley, Matthew J., Drover, Marcus W., & Peters, Jonas C. Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes. United States. https://doi.org/10.1021/acs.chemrev.9b00638
Chalkley, Matthew J., Drover, Marcus W., and Peters, Jonas C. Thu .
"Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes". United States. https://doi.org/10.1021/acs.chemrev.9b00638. https://www.osti.gov/servlets/purl/1698026.
@article{osti_1698026,
title = {Catalytic N2-to-NH3 (or -N2H4) Conversion by Well-Defined Molecular Coordination Complexes},
author = {Chalkley, Matthew J. and Drover, Marcus W. and Peters, Jonas C.},
abstractNote = {Nitrogen fixation, the six-electron/six-proton reduction of N2, to give NH3, is one of the most challenging and important chemical transformations. Notwithstanding the barriers associated with this reaction, significant progress has been made in developing molecular complexes that reduce N2 into its bioavailable form, NH3. This progress is driven by the dual aims of better understanding biological nitrogenases and improving upon industrial nitrogen fixation. In this review, we highlight both mechanistic understanding of nitrogen fixation that has been developed, as well as advances in yields, efficiencies, and rates that make molecular alternatives to nitrogen fixation increasingly appealing. We begin with a historical discussion of N2 functionalization chemistry that traverses a timeline of events leading up to the discovery of the first bona fide molecular catalyst system and follow with a comprehensive overview of d-block compounds that have been targeted as catalysts up to and including 2019. Furthermore, we end with a summary of lessons learned from this significant research effort and last offer a discussion of key remaining challenges in the field.},
doi = {10.1021/acs.chemrev.9b00638},
journal = {Chemical Reviews},
number = 12,
volume = 120,
place = {United States},
year = {Thu Apr 30 00:00:00 EDT 2020},
month = {Thu Apr 30 00:00:00 EDT 2020}
}
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