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<p>Reactive capture – the integration of CO<sub>2</sub> capture with electrochemical upgrade – offers the prospect of improving overall energy efficiency in captured-CO<sub>2</sub>-to-fuels by eliminating the gas-phase CO<sub>2</sub> desorption step, and by further offering a CO<sub>2</sub>-free gas product stream. Two related challenges limit the potential impact of electrified reactive capture today: its propensity to produce lower-value C<sub>1</sub> products (carbon products containing one carbon atom per molecule); and its failure to retain performance when fed dilute streams (e.g. ~1-10% CO<sub>2</sub>). We posit that these could be addressed using catalysts that locally concentrate and activate in-situ generated CO<sub>2</sub>: we integrate a redox-active polymeric network whose polymer fragments undergo reversible reduction during the electrochemical conversion process, enabling electron transfer to CO<sub>2</sub> molecules generated in-situ from carbonate capture liquid. We report as a result a 55 ± 5% C<sub>2+</sub> (carbon products containing two or more carbon atoms per molecule) Faradaic efficiency (FE) at 300 mA/cm<sup>2</sup> in an electrochemical reactive capture system in which the electrolysis stage is fed with 1 M K<sub>2</sub>CO<sub>3</sub>. We obtain 56 ± 4 wt% C<sub>2</sub>H<sub>4</sub> in the product gas stream. When we use a dilute stream consisting of 1% CO<sub>2</sub> in N<sub>2</sub> at the KOH capture stage, we retain the C<sub>2+</sub> FE to within 85% (relative) of its value achieved in the case of pure CO<sub>2</sub>.</p>

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A redox-active polymeric network facilitates electrified reactive-capture electrosynthesis to multi-carbon products from dilute CO2-containing streams

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月15日

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  • Jinqiang Zhang,
  • Yufei Cao,
  • Pengfei Ou,
  • Geonhui Lee,
  • Yufei Zhao,
  • Shijie Liu,
  • Erfan Shirzadi,
  • Roham Dorakhan,
  • Ke Xie,
  • Cong Tian,
  • Yuanjun Chen,
  • Xiaoyan Li,
  • Yurou Celine Xiao,
  • Ali Shayesteh Zeraati,
  • Rui Kai Miao,
  • Sungjin Park,
  • Colin P. O’Brien,
  • Jun Ge,
  • Xin Zhou,
  • David Sinton,
  • Edward H. Sargent

摘要

Reactive capture – the integration of CO2 capture with electrochemical upgrade – offers the prospect of improving overall energy efficiency in captured-CO2-to-fuels by eliminating the gas-phase CO2 desorption step, and by further offering a CO2-free gas product stream. Two related challenges limit the potential impact of electrified reactive capture today: its propensity to produce lower-value C1 products (carbon products containing one carbon atom per molecule); and its failure to retain performance when fed dilute streams (e.g. ~1-10% CO2). We posit that these could be addressed using catalysts that locally concentrate and activate in-situ generated CO2: we integrate a redox-active polymeric network whose polymer fragments undergo reversible reduction during the electrochemical conversion process, enabling electron transfer to CO2 molecules generated in-situ from carbonate capture liquid. We report as a result a 55 ± 5% C2+ (carbon products containing two or more carbon atoms per molecule) Faradaic efficiency (FE) at 300 mA/cm2 in an electrochemical reactive capture system in which the electrolysis stage is fed with 1 M K2CO3. We obtain 56 ± 4 wt% C2H4 in the product gas stream. When we use a dilute stream consisting of 1% CO2 in N2 at the KOH capture stage, we retain the C2+ FE to within 85% (relative) of its value achieved in the case of pure CO2.