<p>Direct air capture of CO<sub>2</sub> often uses alkali hydroxides to form carbonate; however, releasing CO<sub>2</sub> and regenerating alkali hydroxides requires an energy-intensive thermal cycle at ~900 °C. Reactive capture systems instead seek to integrate CO<sub>2</sub> release with its chemical reduction in the pathway to fuels and chemicals. Here we focus on a purely electrosynthetic route, beginning by examining why previous attempts at electrified ethylene synthesis from carbonate post-capture liquids have suffered from low overall energy efficiencies. We find that a hydrophilic environment and limited rate of CO<sub>2</sub> generation in situ lead to low CO<sub>2</sub> availability and consequently low *CO coverage on the catalyst surface, and that this hinders C–C coupling. We identify dilute alloy catalysts that implement asymmetric CO–CHO coupling, a lower-barrier route to C–C coupling compared with the conventional symmetric pathway. We report a 51% ± 2% ethylene Faradaic efficiency, a 66 wt% ± 2% concentrated ethylene stream and a 20% end-to-end energy efficiency at 200 mA cm<sup>−2</sup>. The energy efficiency is a twofold improvement over the most efficient prior report of ethylene production via electrified reactive capture.</p><p></p>

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Dilute alloy electrocatalysts enable asymmetric C–C coupling for ethylene production from a CO2 post-capture liquid

  • Yuanjun Chen,
  • Peiying Wang,
  • Yu Mao,
  • Guangcan Su,
  • Hengzhou Liu,
  • Bosi Peng,
  • Zeyan Liu,
  • Huajie Ze,
  • Yong Wang,
  • Xiaobing Hu,
  • Jiantao Li,
  • Lizhou Fan,
  • Ammar Alahmed,
  • Aqil Jamal,
  • Issam Gereige,
  • Sungsik Lee,
  • Jennifer B. Dunn,
  • Ziyun Wang,
  • Ke Xie,
  • Edward H. Sargent

摘要

Direct air capture of CO2 often uses alkali hydroxides to form carbonate; however, releasing CO2 and regenerating alkali hydroxides requires an energy-intensive thermal cycle at ~900 °C. Reactive capture systems instead seek to integrate CO2 release with its chemical reduction in the pathway to fuels and chemicals. Here we focus on a purely electrosynthetic route, beginning by examining why previous attempts at electrified ethylene synthesis from carbonate post-capture liquids have suffered from low overall energy efficiencies. We find that a hydrophilic environment and limited rate of CO2 generation in situ lead to low CO2 availability and consequently low *CO coverage on the catalyst surface, and that this hinders C–C coupling. We identify dilute alloy catalysts that implement asymmetric CO–CHO coupling, a lower-barrier route to C–C coupling compared with the conventional symmetric pathway. We report a 51% ± 2% ethylene Faradaic efficiency, a 66 wt% ± 2% concentrated ethylene stream and a 20% end-to-end energy efficiency at 200 mA cm−2. The energy efficiency is a twofold improvement over the most efficient prior report of ethylene production via electrified reactive capture.