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<p>CO<sub>2</sub> 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 O<sub>2</sub>, 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 O<sub>2</sub>-sensitive reduced phenazine, enabling stable and effective CO<sub>2</sub> capture from gas mixtures containing O<sub>2</sub>. This flow cell demonstrated substantial oxygen compatibility, exhibiting a coulombic efficiency of 99% and requiring only 73 kJ mol<sup>−1</sup> CO<sub>2</sub> for simulated flue gas and 104 kJ mol<sup>−1</sup> CO<sub>2</sub> 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.</p>

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

  • 期刊论文

  • 发表日期：

    2025年8月22日

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  • Xinyu Jin,
  • Shijian Jin,
  • Lu Li,
  • Roy G. Gordon,
  • Pan Wang,
  • Michael J. Aziz,
  • Yunlong Ji

摘要

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.