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Cobaloximes as Functional Models for Hydrogenases. 2. Proton Electroreduction Catalyzed by Difluoroborylbis(dimethylglyoximato)cobalt(II) Complexes in Organic Media
Abstract
Cobaloximes are effective electrocatalysts for hydrogen evolution and thus functional models for hydrogenases. Among them, difluoroboryl-bridged complexes appear both to mediate proton electroreduction with low overpotentials and to be quite stable in acidic conditions. We report here a mechanistic study of [Co(dmgBF2)2L] (dmg2- = dimethylglyoximato dianion; L = CH3CN or N,N-dimethylformamide) catalyzed proton electroreduction in organic solvents. Depending on the applied potential and the strength of the acid used, three different pathways for hydrogen production were identified and a unified mechanistic scheme involving cobalt(II) or cobalt(III) hydride species is proposed. As far as working potential and turnover frequency are concerned, [Co(dmgBF2)2(CH3CN)2], in the presence of p-cyanoanilinium cation in acetonitrile, is one of the best synthetic catalysts of the first-row transition-metal series for hydrogen evolution.
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Cited by
Chatenet, M., Pollet, B. G., Dekel, D. R., Dionigi, F., Deseure, J., Millet, P., Braatz, R. D., Bazant, M. Z., Eikerling, M., Staffell, I., et al. (2022) · Chemical Society Reviews · doi:10.1039/d0cs01079k · Cited by 2,025
Earth-abundant hydrogen evolution electrocatalysts
McKone, J. R., Marinescu, S. C., Brunschwig, B. S., Winkler, J. R., & Gray, H. B. (2014) · Chem. Sci. · doi:10.1039/c3sc51711j · Cited by 727
Thoi, V. S., Sun, Y., Long, J. R., & Chang, C. J. (2013) · Chem. Soc. Rev. · doi:10.1039/c2cs35272a · Cited by 668
Molecular metal–Nx centres in porous carbon for electrocatalytic hydrogen evolution
Liang, H.-W., Brüller, S., Dong, R., Zhang, J., Feng, X., & Müllen, K. (2015) · Nature Communications · doi:10.1038/ncomms8992 · Cited by 655
Electrocatalytic Hydrogen Evolution in Acidic Water with Molecular Cobalt Tetraazamacrocycles
McCrory, C. C. L., Uyeda, C., & Peters, J. C. (2012) · Journal of the American Chemical Society · doi:10.1021/ja210661k · Cited by 351
Singh, W. M., Baine, T., Kudo, S., Tian, S., Ma, X. A. N., Zhou, H., DeYonker, N. J., Pham, T. C., Bollinger, J. C., Baker, D. L., et al. (2012) · Angewandte Chemie · doi:10.1002/ange.201200082 · Cited by 66
Metadata
- Authors
- Baffert, C., Artero, V., & Fontecave, M.
- Venue
- Inorganic Chemistry
- Publisher
- American Chemical Society (ACS)
- Published
- 2007-02-02
- Volume
- 46
- Issue
- 5
- Pages
- 1817-1824
- ISSN
- 0020-1669 (ISSN-L)
- 1520-510X
- OpenAlex
- W2053956735
- Cited by
- 384
- References
- 0
- FWCI
- 9.71
- Type
- journal article
- Language
- en
- Open access
- closed
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