Publication date: 28th August 2024
Previous electrochemical CO2 reduction studies have shown alkaline electrolytes favor the production of acetaldehyde over acetaldehyde and ethanol, and proposed hypothesis of their generation pathways accordingly [1], [2], [3]. However, our work shows acetate can also come from the fast non-faradaic chemical oxidation of acetaldehyde in alkaline solutions [4]. This could lead to an overestimated acetate productivity and correspondingly an underestimated acetaldehyde productivity, and thus mislead following investigations on the reaction mechanisms of CO2 reduction reaction conducted in alkaline environment.
In the presented work, we will first systematically demonstrate how and why misleading acetaldehyde and acetate production could be caused, and propose suggestions on accurately measuring their productivities in alkaline electrolytes. In addition, we will present real-time detection of gas (hydrogen, methane and ethylene) and volatile liquid (acetaldehyde) being produced during electrochemical CO reduction on polycrystalline and various single crystal ((100), (110), (111), and (211)) Cu electrodes at low overpotentials (< 0.65 V ). Results reveal that acetaldehyde production as well as the production rate of acetaldehyde to ethylene are both potential- and facet-dependent. The quantified acetaldehyde-to-ethylene production ratio will provide insightful information for understanding the bifurcation point of acetaldehyde/ethylene production from electrochemical CO2 reduction in a mechanistic perspective.
B.S. and Y.Q. acknowledge European Union’s Horizon 2020 research and innovation programme under grant agreement no. 85144 (SELECT-CO2), the Villum Center for the Science of Sustainable Fuels and Chemical grant 9455 (VSustain), Carlsberg Foundation (EHALIDE, project no. CF19-02, and Capturing CO2 for simultaneous chlorine and ethanol production using seawater and sustainable electricity grant 1115-00007B (CapCO2). The authors would also like to acknowledge George Kastlunger for useful discussions on reaction mechanisms.
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