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Catalytic Reduction of Dinitrogen to Ammonia at a Single Molybdenum Center
Open accessAbstract
This account explores the catalytic reduction of dinitrogen by molybdenum complexes that contain the [HIPTN(3)N](3-) ligand ([HIPTN(3)N](3-)) = [(HIPTNCH(2)CH(2))(3)N](3-), where HIPT = 3,5-(2,4,6-i-Pr(3)C(6)H(2))(2)C(6)H3) at room temperature and pressure with protons and electrons. A total of 7-8 equiv of ammonia is formed out of approximately 12 possible (depending upon the Mo derivative employed). No hydrazine is formed. Numerous X-ray studies of proposed intermediates in the catalytic cycle suggest that N(2) is being reduced at a sterically protected, single Mo center operating in oxidation states between Mo(III) and Mo(VI). Subtle variations of the [HIPTN(3)N](3-) ligand are not as successful as a consequence of an unknown shunt in the catalytic cycle that consumes reduction equivalents to yield (it is proposed) dihydrogen [corrected]
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Cites
Structure–function relationships of alternative nitrogenases
Eady, R. R. (1996) · Chemical Reviews · doi:10.1021/cr950057h · Cited by 877
Cooperation of GGAs and AP-1 in Packaging MPRs at the Trans-Golgi Network
Doray, B., Ghosh, P., Griffith, J., Geuze, H. J., & Kornfeld, S. (2002) · Science · doi:10.1126/science.1075327 · Cited by 312
Cited by
Mechanism of Nitrogen Fixation by Nitrogenase: The Next Stage
Hoffman, B. M., Lukoyanov, D., Yang, Z.-Y., Dean, D. R., & Seefeldt, L. C. (2014) · Chemical Reviews · doi:10.1021/cr400641x · Cited by 1,766
Can sustainable ammonia synthesis pathways compete with fossil-fuel based Haber–Bosch processes?
Wang, M., Khan, M. A., Mohsin, I., Wicks, J., Ip, A. H., Sumon, K. Z., Dinh, C.-T., Sargent, E. H., Gates, I. D., & Kibria, M. G. (2021) · Energy & Environmental Science · doi:10.1039/d0ee03808c · Cited by 518
McEnaney, J. M., Singh, A. R., Schwalbe, J. A., Kibsgaard, J., Lin, J. C., Cargnello, M., Jaramillo, T. F., & Nørskov, J. K. (2017) · Energy & Environmental Science · doi:10.1039/c7ee01126a · Cited by 474
Metadata
- Authors
- Schrock, R. R.
- Venue
- Accounts of Chemical Research
- Publisher
- American Chemical Society (ACS)
- Published
- 2005-11-10
- Volume
- 38
- Issue
- 12
- Pages
- 955-962
- ISSN
- 0001-4842 (ISSN-L)
- 1520-4898
- OpenAlex
- W3020848186
- Cited by
- 496
- References
- 2
- FWCI
- 11.77
- Type
- journal article
- Language
- en
- Open access
- green
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