Abstract

Surplus renewable electricity used to convert CO2 into CO, the building block of liquid fuels, advances the energy transition by enabling large-scale, long-term energy storage and the synthesis of fuel for long-haul transportation. Among the various technologies developed, renewable electricity driven conversion of CO2 by high-temperature electrolysis and by plasmolysis offer a tantalising potential. High-temperature electrolysis is characterized by high-yield and energy-efficiency and the direct separation of the CO2 dissociation products CO and O2. However, the difficulty to break the carbon-oxygen double bond poses challenging requirements on electrode materials. CO2 plasmolysis on the other hand, offers a similar energy efficiency, does not employ scarce materials, is easy to upscale, but requires efficient gas separation and recuperation because the produced CO remains mixed with O2 and residual CO2. Here, we demonstrate that the coupling of the two processes leads to a renewable-electricity-driven route for producing CO from CO2, overcoming the main bottleneck of CO2 plasmolysis. A simulated CO2 plasmolysis gas mixture is supplied to a high-temperature electrolyser to separate the product gases electrochemically. Our results show that the product stream of the coupled-process contains 91% less oxygen and 138% more CO compared with the bare plasmolysis process. Apart from upgrading the produced gas mixture, this coupled approach benefits from material stability. Durability tests (~100 h) show better stability in coupled operation when compared with conventional CO2 electrolysis. Synergy between plasmolysis and electrolysis opens up a novel route to efficient CO2 conversion into valuable CO feedstock for the synthesis of long-chain hydrocarbons.

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