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://WOS:000331481600003
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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