Bicarbonate Is Not a General Acid in Au-Catalyzed CO₂ Electroreduction
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Author(s)
Wuttig, Anna
Yoon, Youngmin
Ryu, Jaeyune
Surendranath, Yogesh
Date Issued
November 2017
Journal
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
Abstract
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.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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DOI of Published Version
https://doi.org/10.1021/jacs.7b08345
