Bicarbonate Is Not a General Acid in Au-Catalyzed CO₂ Electroreduction
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. Comp...
Главные авторы: | , , , |
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Другие авторы: | |
Формат: | Статья |
Язык: | en_US |
Опубликовано: |
American Chemical Society (ACS)
2018
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Online-ссылка: | http://hdl.handle.net/1721.1/118297 https://orcid.org/0000-0001-9519-7907 https://orcid.org/0000-0002-8683-975X https://orcid.org/0000-0003-1016-3420 |
Итог: | 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. |
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