Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.145
Publication date: 18th December 2023
Carbon dioxide (CO2) exhibits a great potential as the raw reactant for the formation of various carbon-based compounds. Using copper (Cu) as a cathode catalyst in a CO2 electrolyser offers a unique feature of producing multi-carbon products (C2+-products) [1]. The scale up of the CO2 electrolyser technology does require the catalyst activity for these products to remain stable for a high number of operational hours. Despite of this, copper experiences structural changes and , as a result, loss of catalytic activity with time towards ethylene when exposed to a negative potential [2]. Implementing periodic oxidation phases induces formation of cuprite (Cu2O), with other works showing its benefit to the stability of CO2 electrolysis towards C2 products [3]. In this work, different criteria for the (electro)chemical oxidation of copper in a PEEK- flow cell as method of lengthening the catalytic activity are formulated. Using different ‘off’ potential values and different times spend at the open circuit potential (OCP) after a reduction period at 100 mA⋅cm-2, the process of electrochemical and chemical oxidation were studied, respectively. The results show the degree of oxidation during both chemical and electrochemical oxidation to be a determining factor for lengthening the catalyst activity towards ethylene. The latter did show an oxidation period of less than 30 seconds to be sufficient to reach similar effects if an adequate off potential is implemented, whereas chemical oxidation requires 15 minutes to demonstrate the benefits on the stabilization of ethylene selectivity with time. With the oxygen reduction reaction being the cathodic reaction during the chemical oxidation at OCP, additional supply of oxygen into the catholyte’s headspace did result in an accelerated chemical oxidation, reducing the required OCP time from 15 minutes to 5 minutes. In-situ Raman spectroscopy and ex-situ SEM supported the claims made. The gained insights were utilized to conduct a stability test, reaching 15 hours without significant selectivity loss of ethylene.
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