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Catalytic Silylation of Dinitrogen with a Dicobalt Complex
Abstract
A dicobalt complex catalyzes N2 silylation with Me3SiCl and KC8 under 1 atm N2 at ambient temperature. Tris(trimethylsilyl)amine is formed with an initial turnover rate of 1 N(TMS)3/min, ultimately reaching a turnover number of ∼200. The dicobalt species features a metal-metal interaction, which we postulate is important to its function. Although N2 functionalization occurs at a single cobalt site, the second cobalt center modifies the electronics at the active site. Density functional calculations reveal that the Co-Co interaction evolves during the catalytic cycle: weakening upon N2 binding, breaking with silylation of the metal-bound N2 and reforming with expulsion of [N2(SiMe3)3](-).
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Cites
Phenol-hypochlorite reaction for determination of ammonia
Weatherburn, M. W. (1967) · Analytical Chemistry · doi:10.1021/ac60252a045 · Cited by 4,099
Cited by
Electro- and Solar-Driven Fuel Synthesis with First Row Transition Metal Complexes
Dalle, K. E., Warnan, J., Leung, J. J., Reuillard, B., Karmel, I. S., & Reisner, E. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00392 · Cited by 912
Computational Approach to Molecular Catalysis by 3d Transition Metals: Challenges and Opportunities
Vogiatzis, K. D., Polynski, M. V., Kirkland, J. K., Townsend, J., Hashemi, A., Liu, C., & Pidko, E. A. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00361 · Cited by 423
Self-citationDeacy, A. C., Kilpatrick, A. F. R., Regoutz, A., & Williams, C. K. (2020) · Nature Chemistry · doi:10.1038/s41557-020-0450-3 · Cited by 325
Eizawa, A., Arashiba, K., Tanaka, H., Kuriyama, S., Matsuo, Y., Nakajima, K., Yoshizawa, K., & Nishibayashi, Y. (2017) · Nature Communications · doi:10.1038/ncomms14874 · Cited by 257
Metadata
- Authors
- Siedschlag, R. B., Bernales, V., Vogiatzis, K. D., Planas, N., Clouston, L. J., Bill, E., Gagliardi, L., & Lu, C. C.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-04-06
- Volume
- 137
- Issue
- 14
- Pages
- 4638-4641
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2043772300
- Cited by
- 182
- References
- 1
- FWCI
- 10.94
- Type
- journal article
- Language
- en
- Open access
- closed
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- Siedschlag, R. B., Bernales, V., Vogiatzis, K. D., Planas, N., Clouston, L. J., Bill, E., Gagliardi, L., & Lu, C. C. (2015). Catalytic Silylation of Dinitrogen with a Dicobalt Complex. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.5b01445
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Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
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