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<p>Electrified CO<sub>2</sub> capture and release from air offers net-negative emissions, but today’s liquid-carbonate-based systems have a high energy cost (6–10 GJ per ton of CO<sub>2</sub>), and organic sorbents are oxygen sensitive. Here we report electrified CO<sub>2</sub> surface mineralization/demineralization capture/release, wherein an inorganic capture sorbent, MnO<sub>2</sub>, is electrochemically reduced/activated to generate Mn(III), which mineralizes CO<sub>2</sub> to form MnOOCO<sub>2</sub>H (operando Raman); the process is reversed under oxidative potential. This approach is built upon Mn redox reaction that resides within the water-stable bracket, offering tunable driving force (kinetics/productivity) with applied potential (energy). After optimizing the electrochemical protocol, we capture from air (0.04% CO<sub>2</sub> and 21% O<sub>2</sub>) at 4.1 GJ per ton of CO<sub>2</sub>, with capacity and kinetics comparable to prior sorbents, low sensitivity to oxygen/humidity, 80% single-pass CO<sub>2</sub> capture ratio and release under a pure CO<sub>2</sub> carrier gas stream and pressure drop &lt;150 Pa. The system operates &gt;1,000 h with &gt;90% capacity retention and scales to 20 cm<sup>2</sup> without loss; remaining challenges include material utilization, electrolyte, gas flow/pressure drop and CO<sub>2</sub>-purity management.</p>

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Electrified reversible surface mineralization of CO2 for direct air capture

  • 期刊论文

  • 发表日期：

    2026年2月13日

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  • Zeyan Liu,
  • Huajie Ze,
  • Bosi Peng,
  • Charles B. Musgrave III,
  • Mohammad K. Shehab,
  • Hyun Seung Jung,
  • Hengzhou Liu,
  • Kent O. Kirlikovali,
  • William A. Goddard III,
  • Omar K. Farha,
  • Ke Xie,
  • Edward H. Sargent

摘要

Electrified CO2 capture and release from air offers net-negative emissions, but today’s liquid-carbonate-based systems have a high energy cost (6–10 GJ per ton of CO2), and organic sorbents are oxygen sensitive. Here we report electrified CO2 surface mineralization/demineralization capture/release, wherein an inorganic capture sorbent, MnO2, is electrochemically reduced/activated to generate Mn(III), which mineralizes CO2 to form MnOOCO2H (operando Raman); the process is reversed under oxidative potential. This approach is built upon Mn redox reaction that resides within the water-stable bracket, offering tunable driving force (kinetics/productivity) with applied potential (energy). After optimizing the electrochemical protocol, we capture from air (0.04% CO2 and 21% O2) at 4.1 GJ per ton of CO2, with capacity and kinetics comparable to prior sorbents, low sensitivity to oxygen/humidity, 80% single-pass CO2 capture ratio and release under a pure CO2 carrier gas stream and pressure drop <150 Pa. The system operates >1,000 h with >90% capacity retention and scales to 20 cm2 without loss; remaining challenges include material utilization, electrolyte, gas flow/pressure drop and CO2-purity management.