Aromatic Ester-Functionalized Ionic Liquid for Highly Efficient CO2Electrochemical Reduction to Oxalic Acid

被引:40
作者
Yang, Yingliang [1 ,2 ]
Gao, Hongshuai [1 ]
Feng, Jiaqi [1 ,3 ]
Zeng, Shaojuan [1 ]
Liu, Lei [1 ]
Liu, Licheng [4 ,5 ]
Ren, Baozeng [2 ]
Li, Tao [2 ]
Zhang, Suojiang [1 ,3 ]
Zhang, Xiangping [1 ,3 ,5 ]
机构
[1] Chinese Acad Sci, Inst Proc Engn, Beijing Key Lab Ion Liquids Clean Proc, State Key Lab Multiphase Complex Syst, Beijing 100190, Peoples R China
[2] Zhengzhou Univ, Coll Chem Engn, Zhengzhou 450001, Peoples R China
[3] Univ Chinese Acad Sci, Coll Chem Engn, Beijing 100049, Peoples R China
[4] Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, CAS Key Lab Biobased Mat, Qingdao 266101, Peoples R China
[5] Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
基金
国家自然科学基金重大项目; 中国国家自然科学基金; 国家重点研发计划;
关键词
CO(2)reduction; electrocatalyst; electrolysis; ionic liquid; oxalic acid; ELECTROCHEMICAL REDUCTION; CARBON-DIOXIDE; CO2; REDUCTION; OXALATE FORMATION; FORMIC-ACID; CONVERSION; CATALYSIS; CAPTURE;
D O I
10.1002/cssc.202001194
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical reduction of CO(2)into valuable chemicals is a significant route to utilize CO(2)resources. Among various electroreduction products, oxalic acid (H2C2O4) is an important chemical for pharmaceuticals, rare earth extraction, and metal processing. Here, an aprotic aromatic ester-functionalized ionic liquid (IL), 4-(methoxycarbonyl) phenol tetraethylammonium ([TEA][4-MF-PhO]), was designed as an electrolyte for CO(2)electroreduction into oxalic acid. It exhibited a large oxalic acid partial current density of 9.03 mA cm(-2)with a faradaic efficiency (FE) of 86 % at -2.6 V (vs. Ag/Ag+), and the oxalic acid formation rate was as high as 168.4 mu mol cm(-2) h(-1), which is the highest reported value to date. Moreover, the results of density functional theory calculations demonstrated that CO(2)was efficiently activated to a -COOH intermediate by bis-active sites of the aromatic ester anion via the formation of a [4-MF-PhO-COOH](-)adduct, which finally dimerized into oxalic acid.
引用
收藏
页码:4900 / 4905
页数:6
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