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A Highly Stable Rhenium−Cobalt System for Photocatalytic H2 Production: Unraveling the Performance-Limiting Steps
Abstract
Increased long-term performance was found for photocatalytic H(2) production in a homogeneous combination of [Re(NCS)(CO)(3)bipy] (1; bipy = 2,2'-bipyridine), [Co(dmgH)(2)] (dmgH(2) = dimethylglyoxime), triethanolamine (TEOA), and [HTEOA][BF(4)] in N,N-dimethylformamide, achieving TON(Re) up to 6000 (H/Re). The system proceeded by reductive quenching of *1 by TEOA, followed by fast (k(1) = 1.3 x 10(8) M(-1) s(-1)) electron transfer to [Co(II)(dmgH)(2)] and subsequent protonation (K(2)) and elimination (k(3), second-order process in cobalt) of H(2). Observed quantum yields were up to approximately 90% (H produced per absorbed photon). The type of acid had a substantial effect on the long-term stability. A decomposition pathway involving cobalt is limiting the long-term performance. Time-resolved infrared (IR) spectroscopy confirmed that photooxidized TEOA generates a second reducing equivalent, which can be transferred to 1 (70%, k(2e)(-) = 3.3 x 10(8) M(-1) s(-1)) if no [Co(II)(dmgH)(2)] is present.
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Citations
Cited by
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A Cobalt–Dithiolene Complex for the Photocatalytic and Electrocatalytic Reduction of Protons
McNamara, W. R., Han, Z., Alperin, P. J., Brennessel, W. W., Holland, P. L., & Eisenberg, R. (2011) · Journal of the American Chemical Society · doi:10.1021/ja207842r · Cited by 398
Recent developments in hydrogen evolving molecular cobalt(II)–polypyridyl catalysts
Queyriaux, N., Jane, R. T., Massin, J., Artero, V., & Chavarot-Kerlidou, M. (2015) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2015.03.014 · Cited by 274
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Metadata
- Authors
- Probst, B., Rodenberg, A., Guttentag, M., Hamm, P., & Alberto, R.
- Venue
- Inorganic Chemistry
- Publisher
- American Chemical Society (ACS)
- Published
- 2010-06-16
- Volume
- 49
- Issue
- 14
- Pages
- 6453-6460
- ISSN
- 0020-1669 (ISSN-L)
- 1520-510X
- OpenAlex
- W1990241573
- Cited by
- 218
- References
- 0
- FWCI
- 9.78
- Type
- journal article
- Language
- en
- Open access
- closed
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- Probst, B., Rodenberg, A., Guttentag, M., Hamm, P., & Alberto, R. (2010). A Highly Stable Rhenium−Cobalt System for Photocatalytic H2 Production: Unraveling the Performance-Limiting Steps. Inorganic Chemistry. https://doi.org/10.1021/ic100036v
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