Summary Carbon capture and storage, in which CO2 is selectively removed and sequestrated from flue gas, is a promising strategy to mitigate CO2 emissions and global warming. Conventionally, CO2 capture involves an energy-consuming absorbent regeneration step by thermal decomposition (2.0 – 4.0 GJ ton − 1 CO2), which accounts for the majority (60 % – 70 %) of the total cost. Here, we propose an alternative electrochemical cycle to capture CO2 in an aqueous alkaline solution, facilitated by the pH swing effect from a proton-coupled electron transfer redox reaction of a biological proton carrier, riboflavin 5 ′-monophosphate sodium salt hydrate (FMN/FMNH2). Under lab conditions, an electrolysis cell implementing the FMN proton carrier demonstrates a high energy efficiency, with only 9.8 kJ mol − 1 CO2 captured, which is much lower than traditional approaches using a monoethanolamine absorbent (2.0 – 4.0 GJ ton − 1 CO2, 88 – 176 kJ mol − 1 CO2). Thus, this system may contribute toward lowering the cost of CO2 capture.
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