期刊
CHEMSUSCHEM
卷 13, 期 18, 页码 4900-4905出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202001194
关键词
CO(2)reduction; electrocatalyst; electrolysis; ionic liquid; oxalic acid
资金
- National Key R&D Program of China [2018YFB0605802]
- National Natural Science Foundation of China [21838010, 51574215]
- Major Program of National Natural Science Foundation of China [21890760, 21890762]
- Beijing Municipal Natural Science Foundation [2182072, 2182071]
- DNL Cooperation Fund, CAS [DNL 180406]
- Zhengzhou High Level Talent [20180200029]
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.
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