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Aprotic phosphonium-based ionic liquid as electrolyte for highly CO2 electroreduction to oxalate
  • +6
  • Chongyang Jiang,
  • Ma Xifei,
  • Shaojuan Zeng,
  • Feng jiaqi,
  • Li Guilin,
  • Lu Bai,
  • fangfang Li,
  • Xiaoyan Ji,
  • Xiangping Zhang
Chongyang Jiang
Institute of Process Engineering, Chinese Academy of Sciences, Beijing Key Laboratory of Ionic Liquids Clean Process, State Key Laboratory of Multiphase Complex Systems, Key Laboratory of Green Process and Engineering

Corresponding Author:[email protected]

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Shaojuan Zeng
Institute of Process Engineering, Chinese Academy of Sciences
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Feng jiaqi
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Lu Bai
Institute of Process Engineering Chinese Academy of Sciences
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fangfang Li
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Xiaoyan Ji
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Xiangping Zhang
Institute of Process Engineering,CAS
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In this study, a new electrolyte system consisting of tetrabutylphosphonium 4-(methoxycarbonyl) phenol ([P4444][4-MF-PhO]) ionic liquid and acetonitrile (AcN) was developed as CO2 electroreduction electrolyte to produce oxalate, and the mechanism was studied. The results showed that using the new ionic liquid-based electrolyte, the reduction system exhibits 93.8% Faradaic efficiency and 12.6 mA cm-2 partial current density of oxalate at -2.6 V (vs. Ag/Ag+). The formation rate of oxalate is 234.4 μmol cm-2 h-1, which is better than that reported in the literature. The mechanism study using density functional theory (DFT) calculation revealed for the first time that [P4444][4-MF-PhO] IL can effectively activate CO2 molecules through ester and phenoxy double active sites, stabilize the reaction intermediate. The potential barriers of the key intermediates *CO2- and *C2O42- formation by induced electric-field was reduced in the phosphonium-based ionic environment, which greatly facilitates the activation and conversion of CO2 molecules to oxalate.
20 Mar 2022Submitted to AIChE Journal
21 Mar 2022Submission Checks Completed
21 Mar 2022Assigned to Editor
24 Mar 2022Reviewer(s) Assigned
08 May 2022Editorial Decision: Revise Major
03 Jun 20221st Revision Received
07 Jun 2022Submission Checks Completed
07 Jun 2022Assigned to Editor
08 Jun 2022Reviewer(s) Assigned
11 Jul 2022Editorial Decision: Revise Minor
21 Jul 20222nd Revision Received
21 Jul 2022Submission Checks Completed
21 Jul 2022Assigned to Editor
07 Aug 2022Editorial Decision: Accept