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Characterization of an Fe≡N–NH2Intermediate Relevant to Catalytic N2Reduction to NH3
Open accessAbstract
The ability of certain transition metals to mediate the reduction of N2 to NH3 has attracted broad interest in the biological and inorganic chemistry communities. Early transition metals such as Mo and W readily bind N2 and mediate its protonation at one or more N atoms to furnish M(N(x)H(y)) species that can be characterized and, in turn, extrude NH3. By contrast, the direct protonation of Fe-N2 species to Fe(N(x)H(y)) products that can be characterized has been elusive. Herein, we show that addition of acid at low temperature to [(TPB)Fe(N2)][Na(12-crown-4)] results in a new S = 1/2 Fe species. EPR, ENDOR, Mössbauer, and EXAFS analysis, coupled with a DFT study, unequivocally assign this new species as [(TPB)Fe≡N-NH2](+), a doubly protonated hydrazido(2-) complex featuring an Fe-to-N triple bond. This unstable species offers strong evidence that the first steps in Fe-mediated nitrogen reduction by [(TPB)Fe(N2)][Na(12-crown-4)] can proceed along a distal or "Chatt-type" pathway. A brief discussion of whether subsequent catalytic steps may involve early or late stage cleavage of the N-N bond, as would be found in limiting distal or alternating mechanisms, respectively, is also provided.
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Cites
Structure–function relationships of alternative nitrogenases
Eady, R. R. (1996) · Chemical Reviews · doi:10.1021/cr950057h · Cited by 877
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Liu, J.-C., Ma, X.-L., Li, Y., Wang, Y.-G., Xiao, H., & Li, J. (2018) · Nature Communications · doi:10.1038/s41467-018-03795-8 · Cited by 676
Liu, Y., Su, Y., Quan, X., Fan, X., Chen, S., Yu, H., Zhao, H., Zhang, Y., & Zhao, J. (2018) · ACS Catalysis · doi:10.1021/acscatal.7b02165 · Cited by 578
Comprehensive Understanding of the Thriving Ambient Electrochemical Nitrogen Reduction Reaction
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Metadata
- Authors
- Anderson, J. S., Cutsail, G. E., Rittle, J., Connor, B. A., Gunderson, W. A., Zhang, L., Hoffman, B. M., & Peters, J. C.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-06-10
- Volume
- 137
- Issue
- 24
- Pages
- 7803-7809
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W1479896687
- Cited by
- 172
- References
- 1
- FWCI
- 5.67
- Type
- journal article
- Language
- en
- Open access
- green
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- Anderson, J. S., Cutsail, G. E., Rittle, J., Connor, B. A., Gunderson, W. A., Zhang, L., Hoffman, B. M., & Peters, J. C. (2015). Characterization of an Fe≡N–NH2Intermediate Relevant to Catalytic N2Reduction to NH3. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.5b03432
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