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\begin{document}

\title{Aprotic phosphonium-based ionic liquid as electrolyte for highly CO2
electroreduction to oxalate}



\author[1]{Chongyang Jiang}%
\author[2]{Ma Xifei}%
\author[3]{Shaojuan Zeng}%
\author[2]{Feng jiaqi}%
\author[2]{Li Guilin}%
\author[4]{Lu Bai}%
\author[2]{fangfang Li}%
\author[2]{Xiaoyan Ji}%
\author[5]{Xiangping Zhang}%
\affil[1]{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}%
\affil[2]{Affiliation not available}%
\affil[3]{Institute of Process Engineering, Chinese Academy of Sciences}%
\affil[4]{Institute of Process Engineering Chinese Academy of Sciences}%
\affil[5]{Institute of Process Engineering,CAS}%


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  \date{May 27, 2024}


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\begin{abstract}
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 \selectlanguage{greek}μ\selectlanguage{english}mol 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.%
\end{abstract}%



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