Existence of Persistent High Local pH during Electrochemical CO2 Reduction in Densely Buffered Neutral Medium
Kailun Yang a, Recep Kas a, Wilson Smith a
a Delft University of Technology, The Netherlands, Julianalaan, 136, Delft, Netherlands
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe Fall Meeting19 (NFM19)
#SolCat19. (Photo)electrocatalysis for sustainable carbon utilization: mechanisms, methods, and reactor development
Berlin, Germany, 2019 November 3rd - 8th
Organizer: Matthew Mayer
Oral, Kailun Yang, presentation 273
DOI: https://doi.org/10.29363/nanoge.nfm.2019.273
Publication date: 18th July 2019

Electrochemical reduction of carbon dioxide is a promising pathway to store the electricity produced by intermittent renewable energy sources. Recent literature has focused largely on reaction mechanisms and the effect of morphology on the catalytic behavior towards electrochemical CO2 reduction.[1] However, evaluation of the intrinsic performance of the electrocatalysts is hindered by the existence of immense concentration gradients between the electrode surface and bulk solution. In this work, CO2 was electrochemically reduced on both smooth Cu and Cu nanowire electrodes in densely buffered phosphate solutions to mitigate the concentration gradients and evaluate intrinsic activity of electrodes. In-situ surface enhanced infrared absorption spectroscopy (SEIRAS) was used to measure and correlate the local pH and CO2 concentration to the activity of copper electrodes.[2] It is revealed that simply increasing the buffer capacity is not an effective solution to minimize concentration gradients between the bulk and electrode surface on polycrystalline and copper nanowire electrodes. Drastic increase in the hydrogen evolution reaction rates, when compared to CO2 reduction rates, results in breakdown of the buffer in a narrow potential window. These unforeseen results imply that most of the aqueous CO2 electroreduction studies in H-cells were evaluated under mass transport limitations on copper electrodes.

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