Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
DOI: https://doi.org/10.29363/nanoge.nfm.2022.097
Publication date: 11th July 2022
Upgrading processes are required to improve the quality of raw bio-oil and thereby increase their viability of bio-based fuel usage. Electrochemical upgrading of bio-oil can be an appealing alternative to current upgrading technologies, as they operate at moderate reaction conditions and can employ the expected surplus in electricity due to increasing capacities of renewable energy installations. One way to lower the acid content in bio-oil and thereby improving the quality of the bio-oil is by Kolbe electrolysis. In Kolbe electrolysis, acids are converted to (non)-Kolbe products and carbon dioxide. The reaction conditions strongly influence the product distribution. The influence of electrolyte pH is studied in literature, however its effect on the product outcome is not yet fully resolved. Contradictory observations and conclusions with respect to performance stability have been reported. Therefore, this work investigates the influence of electrolyte pH on the reaction-time and pH dependent product selectivity during Kolbe electrolysis of acetic acid on platinum.
In this study Kolbe electrolysis of acetic acid on a platinum anode in aqueous electrolytes is addressed with a particular focus on electrolyte composition. We will first disclose that a pH similar to, or larger than the pKa of acetic acid is required to favor formation and homocoupling of methyl radicals towards the Kolbe product ethane. However, extended duration of electrolysis of acetate at basic pH results in loss of Faradaic efficiency to the Kolbe product (ethane), compensated by the formation of the Hofer-Moest product (methanol). We postulate that the observed change in selectivity is caused by the dissolution of CO2, resulting in enlarged concentration of (bi)carbonate near the electrode electrolyte interface. During the presentation we present our current understanding of the electrode-electrolyte interface and we will provide evidence that the spatial spacing between two methyl radicals is increased which lowers the dimerization rate. Finally, we will discuss the implications of our observations for practical applications, like bio-oil upgrading.
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