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Electrocatalytic Carbon Dioxide Activation: The Rate‐Determining Step of Pyridinium‐Catalyzed CO2 Reduction
Abstract
The reactivity of reduced pyridinium with CO 2 was investigated as a function of catalyst concentration, temperature, and pressure at platinum electrodes. Concentration experiments show that the catalytic current measured by cyclic voltammetry increases linearly with pyridinium and CO 2 concentrations; this indicates that the rate‐determining step is first order in both. The formation of a carbamate intermediate is supported by the data presented. Increased electron density at the pyridyl nitrogen upon reduction, as calculated by DFT, favors a Lewis acid/base interaction between the nitrogen and the CO 2. The rate of the known side reaction, pyridinium coupling to form hydrogen, does not vary over the temperature range investigated and had a rate constant of 2.5 M−1 s−1. CO 2 reduction followed Arrhenius behavior and the activation energy determined by electrochemical simulation was (69±10) kJ mol−1.
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Cited by
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
Self-citationEnhanced electrocatalytic CO2 reduction via field-induced reagent concentration
Liu, M., Pang, Y., Zhang, B., De Luna, P., Voznyy, O., Xu, J., Zheng, X., Dinh, C. T., Fan, F., Cao, C., et al. (2016) · Nature · doi:10.1038/nature19060 · Cited by 2,000
Kondratenko, E. V., Mul, G., Baltrusaitis, J., Larrazábal, G. O., & Pérez-Ramírez, J. (2013) · Energy & Environmental Science · doi:10.1039/c3ee41272e · Cited by 1,802
Ionic Liquid–Mediated Selective Conversion of CO 2 to CO at Low Overpotentials
Rosen, B. A., Salehi-Khojin, A., Thorson, M. R., Zhu, W., Whipple, D. T., Kenis, P. J. A., & Masel, R. I. (2011) · Science · doi:10.1126/science.1209786 · Cited by 1,558
Recycling of carbon dioxide to methanol and derived products – closing the loop
Goeppert, A., Czaun, M., Jones, J.-P., Surya Prakash, G. K., & Olah, G. A. (2014) · Chem. Soc. Rev. · doi:10.1039/c4cs00122b · Cited by 1,528
Metadata
- Authors
- Morris, A. J., McGibbon, R. T., & Bocarsly, A. B.
- Venue
- ChemSusChem
- Publisher
- Wiley
- Published
- 2011-02-16
- Volume
- 4
- Issue
- 2
- Pages
- 191-196
- ISSN
- 1864-5631 (ISSN-L)
- 1864-564X
- OpenAlex
- W2119942754
- Cited by
- 161
- References
- 0
- FWCI
- 7.09
- Type
- journal article
- Language
- en
- Open access
- closed
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- Morris, A. J., McGibbon, R. T., & Bocarsly, A. B. (2011). Electrocatalytic Carbon Dioxide Activation: The Rate‐Determining Step of Pyridinium‐Catalyzed CO2 Reduction. ChemSusChem. https://doi.org/10.1002/cssc.201000379
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