Bicarbonate Is Not a General Acid in Au-Catalyzed CO₂ Electroreduction
Author(s)
Wuttig, Anna; Yoon, Youngmin; Ryu, Jaeyune; Surendranath, Yogesh
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We show that bicarbonate is neither a general acid nor a reaction partner in the rate-limiting step of electrochemical CO₂ 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 CO₂-saturated aqueous electrolytes.
Date issued
2017-11Department
Massachusetts Institute of Technology. Department of ChemistryJournal
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Citation
Wuttig, Anna et al. “Bicarbonate Is Not a General Acid in Au-Catalyzed CO₂ Electroreduction.” Journal of the American Chemical Society 139, 47 (November 2017): 17109–17113 © 2017 American Chemical Society
Version: Author's final manuscript
ISSN
0002-7863
1520-5126