Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.109
Publication date: 18th July 2023
Carbon dioxide (CO2) electrolysis to produce hydrocarbons and oxygenates using copper (Cu) based catalysts has attracted substantial interest due to the direct production of versatile C2+ feedstocks . Inside the reactor, however, CO2 electrolyzers produce C2+ compounds occur via a two-step tandem CO2 to CO and CO to C2+ steps. Such knowledge has been utilized in catalyst and cathode-to-anode reactor design, but sparingly in the in-plane design of the system. Here we use the knowledge that CO2 reduction on copper is primarily a tandem reaction, and through modulation of the reactor flow rate achieve C2+ selectivity 84% at CO2 utilizations of 31%, exceeding theoretical CO2 utilization efficiencies of 25% for C2+ products. We show that higher utilizations are possible when a subset of the reactor performing only CO reduction, instead of CO2 reduction, preventing excess CO2 conversion to carbonates. Through use of varied flow field (serpentine, parallel, interdigitated) and pure CO-fed electrolysis, we link these our results to CO residence time. Notably we find that while ethylene production is constant with flow rate (~40%), oxygenates increase substantially at lower flow rates, reaching 45% at 10 SCCM. Finally, we posit that researchers should switch to combined ethylene + ethanol selectivity as a qualifying metric due to the ease of dehydrating ethanol to form ethylene and a demonstrated inability to fully control ethylene:oxygenate branching pathways. Efforts should then shift to the removal of ethanol from membrane electrode assembly systems and downstream recovery through existing commercial processes.
The author would like to acknowledge the co-financing provided by Shell and a PPP-allowance from Top Consortia for Knowledge and Innovation (TKI’s) of the Ministry of Economic Affairs and Climate in the context of the TU Delft e-Refinery Institute.
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