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Re(bipy-tBu)(CO)3Cl−improved Catalytic Activity for Reduction of Carbon Dioxide: IR-Spectroelectrochemical and Mechanistic Studies
Abstract
Five Re(bipy)(CO)(3)Cl complexes were prepared and studied where bipy was 4,4'-dicarboxyl-2,2'-bipyridine (1), 2,2'-bipyridine (2), 4,4'-dimethyl-2,2'-bipyridine (3), 4,4'-di-tert-butyl-2,2'-bipyridine (4), and 4,4'-dimethoxy-2,2'-bipyridine (5). From this group, a significantly improved catalyst, Re(bipy-tBu)(CO)(3)Cl (4), for the reduction of carbon dioxide to carbon monoxide was found. The complex shows two one-electron reductions under argon, one reversible at -1445 mV (vs SCE), and one irreversible at -1830 mV. Under CO(2) the second irreversible wave displays a large catalytic enhancement in current. Diffusion coefficients were determined using the Levich-Koutecky method (1.1 × 10(-5) cm(2)/s for the neutral complex and 8.1 × 10(-6) cm(2)/s for the singly reduced species), and a second order rate constant for the electrochemical reduction with CO(2) of 1000 M(-1) s(-1) was measured. Bulk electrolysis studies were performed to measure Faradaic efficiencies for the primary gaseous products, η(CO) = 99 ± 2% in acetonitrile.
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Cited by
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels
Qiao, J., Liu, Y., Hong, F., & Zhang, J. (2014) · Chem. Soc. Rev. · doi:10.1039/c3cs60323g · Cited by 2,990
Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO 2 Fixation
Appel, A. M., Bercaw, J. E., Bocarsly, A. B., Dobbek, H., DuBois, D. L., Dupuis, M., Ferry, J. G., Fujita, E., Hille, R., Kenis, P. J. A., et al. (2013) · Chemical Reviews · doi:10.1021/cr300463y · Cited by 2,193
Molecular polypyridine-based metal complexes as catalysts for the reduction of CO2
Elgrishi, N., Chambers, M. B., Wang, X., & Fontecave, M. (2017) · Chemical Society Reviews · doi:10.1039/c5cs00391a · Cited by 555
Advances in molecular photocatalytic and electrocatalytic CO2 reduction
Windle, C. D., & Perutz, R. N. (2012) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2012.03.010 · Cited by 481
Sampson, M. D., Nguyen, A. D., Grice, K. A., Moore, C. E., Rheingold, A. L., & Kubiak, C. P. (2014) · Journal of the American Chemical Society · doi:10.1021/ja501252f · Cited by 466
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Metadata
- Authors
- Smieja, J. M., & Kubiak, C. P.
- Venue
- Inorganic Chemistry
- Publisher
- American Chemical Society (ACS)
- Published
- 2010-09-16
- Volume
- 49
- Issue
- 20
- Pages
- 9283-9289
- ISSN
- 0020-1669 (ISSN-L)
- 1520-510X
- OpenAlex
- W2036452223
- Cited by
- 535
- References
- 0
- FWCI
- 9.64
- Type
- journal article
- Language
- en
- Open access
- closed
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- Smieja, J. M., & Kubiak, C. P. (2010). Re(bipy-tBu)(CO)3Cl−improved Catalytic Activity for Reduction of Carbon Dioxide: IR-Spectroelectrochemical and Mechanistic Studies. Inorganic Chemistry. https://doi.org/10.1021/ic1008363
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