Highly efficient synthesis of diethyl carbonate via one-pot reaction from carbon dioxide, epoxides and ethanol over KI-based binary catalyst system | |
Wang, Liguo1; Li, Huiquan1; Xin, Shumin1; He, Peng1; Cao, Yan1; Li, Fengjiao1,2; Hou, Xinjuan1 | |
刊名 | APPLIED CATALYSIS A-GENERAL |
2014-02-10 | |
卷号 | 471期号:1页码:19-27 |
关键词 | Diethyl carbonate Ethanol Carbon dioxide Binary catalyst system |
ISSN号 | 0926-860X |
其他题名 | Appl. Catal. A-Gen. |
中文摘要 | The synthesis of diethyl carbonate (DEC) directly from carbon dioxide, ethylene oxide (EO), and ethanol via one-pot reaction is reported for the first time. The effects of catalyst species and reaction variables on the synthetic performance of DEC were systematically studied. The integration of easily available KI and sodium ethoxide as homogeneous binary catalyst system was found to be very active for the one-pot reaction, and 63.6% of the DEC yield could be achieved under relatively mild reaction conditions (443 K, 3 MPa CO2 initial pressure, 2 h). The byproduct of 2-ethoxyethanol, which is predominantly formed via alcoholysis of EO by ethanol through ring-opening reaction, was produced with small amount (<5%) under optimized conditions. Additionally, the thermodynamic evaluation reveals that the standard molar enthalpy of one-pot reaction is exothermic (Delta H-r(m)theta = -19.70 kcal/mol < 0). In comparison with the direct synthesis of DEC from CO2 and ethanol, the involvement of EO facilitates the formation of DEC, simultaneously with glycol produced. This strategy could also be successfully expanded to terminal epoxide substrates. Furthermore, a possible mechanism of the reaction was proposed on the basis of experimental results. This method provides a highly effective way to produce DEC via directly chemical utilization of CO2 and shows promising application in the manufacture of diethyl carbonate on an industrial scale. (C) 2013 Elsevier B.V. All rights reserved. |
英文摘要 | The synthesis of diethyl carbonate (DEC) directly from carbon dioxide, ethylene oxide (EO), and ethanol via one-pot reaction is reported for the first time. The effects of catalyst species and reaction variables on the synthetic performance of DEC were systematically studied. The integration of easily available KI and sodium ethoxide as homogeneous binary catalyst system was found to be very active for the one-pot reaction, and 63.6% of the DEC yield could be achieved under relatively mild reaction conditions (443 K, 3 MPa CO2 initial pressure, 2 h). The byproduct of 2-ethoxyethanol, which is predominantly formed via alcoholysis of EO by ethanol through ring-opening reaction, was produced with small amount (<5%) under optimized conditions. Additionally, the thermodynamic evaluation reveals that the standard molar enthalpy of one-pot reaction is exothermic (Delta H-r(m)theta = -19.70 kcal/mol < 0). In comparison with the direct synthesis of DEC from CO2 and ethanol, the involvement of EO facilitates the formation of DEC, simultaneously with glycol produced. This strategy could also be successfully expanded to terminal epoxide substrates. Furthermore, a possible mechanism of the reaction was proposed on the basis of experimental results. This method provides a highly effective way to produce DEC via directly chemical utilization of CO2 and shows promising application in the manufacture of diethyl carbonate on an industrial scale. (C) 2013 Elsevier B.V. All rights reserved. |
WOS标题词 | Science & Technology ; Physical Sciences ; Life Sciences & Biomedicine |
类目[WOS] | Chemistry, Physical ; Environmental Sciences |
研究领域[WOS] | Chemistry ; Environmental Sciences & Ecology |
关键词[WOS] | METAL-OXIDE CATALYSTS ; DIMETHYL CARBONATE ; ORGANIC CARBONATES ; DIALKYL CARBONATES ; PROPYLENE-OXIDE ; ETHYLENE-OXIDE ; BUTYLENE OXIDE ; CO2 ; METHANOL ; TRANSESTERIFICATION |
收录类别 | SCI |
原文出处 | |
语种 | 英语 |
WOS记录号 | WOS:000331481600003 |
公开日期 | 2014-05-06 |
内容类型 | 期刊论文 |
版本 | 出版稿 |
源URL | [http://ir.ipe.ac.cn/handle/122111/8114] |
专题 | 过程工程研究所_研究所(批量导入) |
作者单位 | 1.Chinese Acad Sci, Inst Proc & Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
推荐引用方式 GB/T 7714 | Wang, Liguo,Li, Huiquan,Xin, Shumin,et al. Highly efficient synthesis of diethyl carbonate via one-pot reaction from carbon dioxide, epoxides and ethanol over KI-based binary catalyst system[J]. APPLIED CATALYSIS A-GENERAL,2014,471(1):19-27. |
APA | Wang, Liguo.,Li, Huiquan.,Xin, Shumin.,He, Peng.,Cao, Yan.,...&Hou, Xinjuan.(2014).Highly efficient synthesis of diethyl carbonate via one-pot reaction from carbon dioxide, epoxides and ethanol over KI-based binary catalyst system.APPLIED CATALYSIS A-GENERAL,471(1),19-27. |
MLA | Wang, Liguo,et al."Highly efficient synthesis of diethyl carbonate via one-pot reaction from carbon dioxide, epoxides and ethanol over KI-based binary catalyst system".APPLIED CATALYSIS A-GENERAL 471.1(2014):19-27. |
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