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<p>Electrochemical CO<sub>2</sub> conversion offers a direct route to decarbonized fuels, but its deployment on industrial flue gas remains hindered by the low CO<sub>2</sub> content, high O<sub>2</sub> levels, and the resulting parasitic oxygen reduction. Binary solvent electrolytes offer a lever to tune the local reaction environment under such dilute and impurity-rich conditions. Here we show a direct reactive capture (DRC) strategy that converts CO<sub>2</sub> from dilute streams into CO with near-quantitative Faradaic efficiency in organic electrolytes under moderate pressure. We identify hydrogen-bond donation ability (HBD) as a decisive parameter governing competing hydrogen evolution and oxygen reduction reactions. Employing low-HBD electrolytes disrupts the hydrogen-bond network, suppresses competing reactions, and enables selective CO<sub>2</sub> conversion even at 1% CO<sub>2</sub> in the presence of O<sub>2</sub>. When fed with 15% CO<sub>2</sub> and 8% O<sub>2</sub> balanced with N<sub>2</sub>, the optimized system sustains &gt;100 h operation with an energy consumption of 30.7 GJ ton<sup>−1</sup> CO, and achieves a solar-to-fuel efficiency of ~5.5%. This impurity-tolerant strategy addresses a key barrier for industrial CO<sub>2</sub> electrolysis and establishes a scalable route to solar-driven fuel production directly from flue gas.</p>

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Hydrogen bond network disruption enables efficient direct reactive capture of CO2 from flue gas

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月7日

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  • Jiefeng Liu,
  • Xiaowan Bai,
  • Zakaria Anfar,
  • Eddy Petit,
  • Mathilde Moderne,
  • Ji Li,
  • Wensen Wang,
  • Chrystelle Salameh,
  • Huali Wu,
  • Yan Jiao,
  • Damien Voiry

摘要

Electrochemical CO2 conversion offers a direct route to decarbonized fuels, but its deployment on industrial flue gas remains hindered by the low CO2 content, high O2 levels, and the resulting parasitic oxygen reduction. Binary solvent electrolytes offer a lever to tune the local reaction environment under such dilute and impurity-rich conditions. Here we show a direct reactive capture (DRC) strategy that converts CO2 from dilute streams into CO with near-quantitative Faradaic efficiency in organic electrolytes under moderate pressure. We identify hydrogen-bond donation ability (HBD) as a decisive parameter governing competing hydrogen evolution and oxygen reduction reactions. Employing low-HBD electrolytes disrupts the hydrogen-bond network, suppresses competing reactions, and enables selective CO2 conversion even at 1% CO2 in the presence of O2. When fed with 15% CO2 and 8% O2 balanced with N2, the optimized system sustains >100 h operation with an energy consumption of 30.7 GJ ton−1 CO, and achieves a solar-to-fuel efficiency of ~5.5%. This impurity-tolerant strategy addresses a key barrier for industrial CO2 electrolysis and establishes a scalable route to solar-driven fuel production directly from flue gas.