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Redox-Switched Oxidation of Dihydrogen Using a Non-Innocent Ligand
Abstract
Organometallic complexes containing non-innocent ligands of the type Cp*Ir(tBAFPh)(1), where H2tBAFPh is 2-(2-trifluoromethyl)anilino-4,6-di-tert-butylphenol, were found to activate H2 in a redox-switchable manner. The 16e- complex 1 was inert with respect to H2, CO, as well as conventional basic substrates until oxidation. Oxidation of 16-electron 1 with 1 equiv of Ag+ resulted in ligand-centered oxidation affording salts of [1]+, which were characterized by crystallographically, EPR, and elemental analyses. [1]+ was reduced to 1 in the presence of H2 and the sterically hindered base, 2,6-(tBu)2C5H3N, via a pathway that is first-order in both metal and dihydrogen. Compound [1]+ forms adducts with MeCN, which inhibits catalysis. The catalytic oxidation of H2 was established by electrochemical methods to be associated with the monocation.
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Cited by
A Biomimetic Copper Water Oxidation Catalyst with Low Overpotential
Zhang, T., Wang, C., Liu, S., Wang, J.-L., & Lin, W. (2014) · Journal of the American Chemical Society · doi:10.1021/ja409267p · Cited by 389
Wang, X., Thevenon, A., Brosmer, J. L., Yu, I., Khan, S. I., Mehrkhodavandi, P., & Diaconescu, P. L. (2014) · Journal of the American Chemical Society · doi:10.1021/ja505883u · Cited by 263
Metadata
- Authors
- Ringenberg, M. R., Kokatam, S. L., Heiden, Z. M., & Rauchfuss, T. B.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2007-12-29
- Volume
- 130
- Issue
- 3
- Pages
- 788-789
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2000578098
- Cited by
- 193
- References
- 0
- FWCI
- 6.97
- Type
- journal article
- Language
- en
- Open access
- closed
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- Ringenberg, M. R., Kokatam, S. L., Heiden, Z. M., & Rauchfuss, T. B. (2008). Redox-Switched Oxidation of Dihydrogen Using a Non-Innocent Ligand. Journal of the American Chemical Society. https://doi.org/10.1021/ja076801k
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