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Bicarbonate Is Not a General Acid in Au-Catalyzed CO2 Electroreduction
Open accessAbstract
We show that bicarbonate is neither a general acid nor a reaction partner in the rate-limiting step of electrochemical CO 2 reduction catalysis mediated by planar polycrystalline Au surfaces. We formulate microkinetic models and propose diagnostic criteria to distinguish the role of bicarbonate. Comparing these models with the observed zero-order dependence in bicarbonate and simulated interfacial concentration gradients, we conclude that bicarbonate is not a general acid cocatalyst. Instead, it acts as a viable proton donor past the rate-limiting step and a sluggish buffer that maintains the bulk but not local pH in CO 2 -saturated aqueous electrolytes.
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How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels
Peterson, A. A., Abild-Pedersen, F., Studt, F., Rossmeisl, J., & Nørskov, J. K. (2010) · Energy & Environmental Science · doi:10.1039/c0ee00071j · Cited by 3,784
Active and Selective Conversion of CO 2 to CO on Ultrathin Au Nanowires
Zhu, W., Zhang, Y.-J., Zhang, H., Lv, H., Li, Q., Michalsky, R., Peterson, A. A., & Sun, S. (2014) · Journal of the American Chemical Society · doi:10.1021/ja5095099 · Cited by 860
Real-Time Observation of Carbonic Acid Formation in Aqueous Solution
Adamczyk, K., Prémont-Schwarz, M., Pines, D., Pines, E., & Nibbering, E. T. J. (2009) · Science · doi:10.1126/science.1180060 · Cited by 315
Cited by
Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte
Nitopi, S., Bertheussen, E., Scott, S. B., Liu, X., Engstfeld, A. K., Horch, S., Seger, B., Stephens, I. E. L., Chan, K., Hahn, C., et al. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00705 · Cited by 5,223
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Birdja, Y. Y., Pérez-Gallent, E., Figueiredo, M. C., Göttle, A. J., Calle-Vallejo, F., & Koper, M. T. M. (2019) · Nature Energy · doi:10.1038/s41560-019-0450-y · Cited by 2,747
Electrocatalysis for CO 2 conversion: from fundamentals to value-added products
Wang, G., Chen, J., Ding, Y., Cai, P., Yi, L., Li, Y., Tu, C., Hou, Y., Wen, Z., & Dai, L. (2021) · Chemical Society Reviews · doi:10.1039/d0cs00071j · Cited by 1,295
Garg, S., Li, M., Weber, A. Z., Ge, L., Li, L., Rudolph, V., Wang, G., & Rufford, T. E. (2020) · Journal of Materials Chemistry A · doi:10.1039/c9ta13298h · Cited by 478
Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts
Sun, L., Reddu, V., Fisher, A. C., & Wang, X. (2020) · Energy & Environmental Science · doi:10.1039/c9ee03660a · Cited by 452
Metadata
- Authors
- Wuttig, A., Yoon, Y., Ryu, J., & Surendranath, Y.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-11-16
- Volume
- 139
- Issue
- 47
- Pages
- 17109-17113
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2764155932
- Cited by
- 263
- References
- 3
- FWCI
- 6.48
- Type
- journal article
- Language
- en
- Open access
- green
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