Published January 16, 2013
| Version Accepted Version + Supplemental Material
Journal Article
Open
Conversion of Fe−NH_2 to Fe−N_2 with release of NH_3
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1.
California Institute of Technology
Abstract
Tris(phosphine)borane ligated Fe(I) centers featuring N_2H_4, NH_3, NH_2, and OH ligands are described. Conversion of Fe–NH_2 to Fe–NH_3^+ by the addition of acid, and subsequent reductive release of NH_3 to generate Fe–N_2, is demonstrated. This sequence models the final steps of proposed Fe–mediated nitrogen fixation pathways. The five-coordinate trigonal bipyramidal complexes described are unusual in that they adopt S = 3/2 ground states and are prepared from a four-coordinate, S = 3/2 trigonal pyramidal precursor.
Additional Information
© 2012 American Chemical Society. Received: August 3, 2012. Published: December 21, 2012. The authors declare no competing financial interest. This work was supported by the NIH (GM 070757) and the Gordon and Betty Moore Foundation, and through the NSF via a GRFP award to J.S.A. M.-E. M. acknowledges a Fellowship for Advanced Researchers from the Swiss National Science Foundation. Larry Henling and Dr. Jens Kaiser are thanked for their assistance with X-ray crystallography and Dr. Angelo DiBilio for his assistance with EPR measurements. We acknowledge the Gordon and Betty Moore Foundation, the Beckman Institute, and the Sanofi-Aventis BRP at Caltech for their generous support of the Molecular Observatory at Caltech. SSRL is operated for the DOE and supported by its Office of Biological and Environmental Research, and by the NIH, NIGMS (including P41GM103393), and the NCRR (P41RR001209).Attached Files
Accepted Version - nihms433859.pdf
Supplemental Material - ja307714m_si_001.pdf
Supplemental Material - ja307714m_si_002.txt
Files
ja307714m_si_001.pdf
Additional details
Identifiers
- PMCID
- PMC3565533
- Eprint ID
- 37155
- DOI
- 10.1021/ja307714m
- Resolver ID
- CaltechAUTHORS:20130226-145140419
Related works
- Describes
- 10.1021/ja307714m (DOI)
Funding
- NIH
- GM 070757
- Gordon and Betty Moore Foundation
- NSF Graduate Research Fellowship
- Swiss National Science Foundation (SNSF)
- Caltech Beckman Institute
- Caltech Sanofi-Aventis Bioengineering Research Program
- Department of Energy (DOE)
- NIH
- P41GM103393
- NIH
- P41RR001209
Dates
- Created
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2013-02-26Created from EPrint's datestamp field
- Updated
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2021-11-09Created from EPrint's last_modified field