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The Homogeneous Reduction of CO2 by [Ni(cyclam)]+: Increased Catalytic Rates with the Addition of a CO Scavenger
Abstract
The homogeneous electrochemical reduction of CO2 by the molecular catalyst [Ni(cyclam)](2+) is studied by electrochemistry and infrared spectroelectrochemistry. The electrochemical kinetics are probed by varying CO2 substrate and proton concentrations. Products of CO2 reduction are observed in infrared spectra obtained from spectroelectrochemical experiments. The two major species observed are a Ni(I) carbonyl, [Ni(cyclam)(CO)](+), and a Ni(II) coordinated bicarbonate, [Ni(cyclam)(CO2OH)](+). The rate-limiting step during electrocatalysis is determined to be CO loss from the deactivated species, [Ni(cyclam)(CO)](+), to produce the active catalyst, [Ni(cyclam)](+). Another macrocyclic complex, [Ni(TMC)](+), is deployed as a CO scavenger in order to inhibit the deactivation of [Ni(cyclam)](+) by CO. Addition of the CO scavenger is shown to dramatically increase the catalytic current observed for CO2 reduction. Evidence for the [Ni(TMC)](+) acting as a CO scavenger includes the observation of [Ni(TMC)(CO)](+) by IR. Density functional theory (DFT) calculations probing the optimized geometry of the [Ni(cyclam)(CO)](+) species are also presented.
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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
Hori, Y., Wakebe, H., Tsukamoto, T., & Koga, O. (1994) · Electrochimica Acta · doi:10.1016/0013-4686(94)85172-7 · Cited by 2,140
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Boutin, E., Merakeb, L., Ma, B., Boudy, B., Wang, M., Bonin, J., Anxolabéhère-Mallart, E., & Robert, M. (2020) · Chemical Society Reviews · doi:10.1039/d0cs00218f · Cited by 423
Chen, L., Guo, Z., Wei, X.-G., Gallenkamp, C., Bonin, J., Anxolabéhère-Mallart, E., Lau, K.-C., Lau, T.-C., & Robert, M. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b06535 · Cited by 359
Metadata
- Authors
- Froehlich, J. D., & Kubiak, C. P.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2015-03-05
- Volume
- 137
- Issue
- 10
- Pages
- 3565-3573
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2325384140
- Cited by
- 253
- References
- 3
- FWCI
- 8.02
- Type
- journal article
- Language
- en
- Open access
- closed
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- Froehlich, J. D., & Kubiak, C. P. (2015). The Homogeneous Reduction of CO2 by [Ni(cyclam)]+: Increased Catalytic Rates with the Addition of a CO Scavenger. Journal of the American Chemical Society. https://doi.org/10.1021/ja512575v
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