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Direct air capture of CO2 in an electrochemical hybrid flow cell with a spatially isolated phenazine electrode

Xinyu Jin, Shijian Jin, Lu Li, Roy G. Gordon, Pan Wang (), Michael J. Aziz () and Yunlong Ji ()
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Xinyu Jin: University of Chinese Academy of Sciences
Shijian Jin: Harvard University
Lu Li: Westlake University
Roy G. Gordon: Harvard University
Pan Wang: Westlake University
Michael J. Aziz: Harvard University
Yunlong Ji: University of Chinese Academy of Sciences

Nature Energy, 2025, vol. 10, issue 9, 1146-1154

Abstract: Abstract CO2 capture based on a pH swing driven electrically through the reversible proton-coupled electron transfer of organic molecules could be powered entirely by clean electricity. A major technical challenge is the reversible chemical oxidation of the reduced organics by atmospheric O2, which can lower energy efficiency and capture capacity. Here we report the development of a hybrid phenazine flow cell system that uses a pH-swing direct air capture (DAC) process, utilizing redox-active cyclic poly(phenazine sulfide) fabricated solid electrodes. The system maintains a separation between the air and the O2-sensitive reduced phenazine, enabling stable and effective CO2 capture from gas mixtures containing O2. This flow cell demonstrated substantial oxygen compatibility, exhibiting a coulombic efficiency of 99% and requiring only 73 kJ mol−1 CO2 for simulated flue gas and 104 kJ mol−1 CO2 for DAC. The strategy of isolating vulnerable species offers an efficient pathway for DAC and may be broadly applicable to avoiding undesirable side reactions in other electrochemical devices.

Date: 2025
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DOI: 10.1038/s41560-025-01836-3

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