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Highly synergistic effect of ionic liquids and Zn-based catalysts for synthesis of cyclic carbonates from urea and diols
Deng, Lili2,3; Sun, Wenzhong1,3; Shi, Zijie2,3; Qian, Wei2,3; Su, Qian3,4; Dong, Li3,4; He, Hongyan3; Li, Zengxi2,3; Cheng, Weiguo3,4
刊名JOURNAL OF MOLECULAR LIQUIDS
2020-10-10
卷号316页码:12
关键词Ionic liquids Catalysts Synergistic effect Urea Cyclic carbonates
ISSN号0167-7322
DOI10.1016/j.molliq.2020.113883
英文摘要The development of stable and efficient catalysts is an attractive topic for green chemistry reactions under mild reaction conditions. In order to improve solvent-free synthesis of cyclic carbonates from urea and diols, a binary catalyst systems of Zn-based and different ionic liquids (ILs) were developed and examined in this study. The yield of ethylene carbonate (EC) could reach to 92.2% in the presence of C(16)mimCl/ZnCl2 catalyst. Through exploring the structure-activity relationships of cation and anion, it was confirmed that a synergistic effect of cation and anion of catalyst had important influences on urea alcoholysis. Additionally, the controlling step of EC synthesis reaction involving the elimination of an ammonia molecule from intermediates had been revealed by in situ FrIR. This could afford a guided insight for synthesizing cyclic carbonates with high yield. Furthermore, a possible mechanism for the catalytic process was proposed based on DFT and the experimental results via FT-IR, H-1 NMR and C-13 NMR analysis, which revealed that not only a probable synergistic effects of cation-anion matters, but also C(2)-H of ifs and Zn2+ played a key role in accelerating the reaction of urea alcoholysis. This catalytic mechanism study is to provide a preliminary basis to develop novel catalysts for cyclic carbonates from urea and diols through a green synthetic pathway. (C) 2020 Published by Elsevier B.V.
资助项目Innovation Academy for Green Manufacture, Chinese Academy of Sciences[IAGM-2019-A01] ; "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences[XDA 21030500] ; National Natural Science Foundation of China[21890763] ; National Natural Science Foundation of China[21908226]
WOS关键词PROPYLENE CARBONATE ; ETHYLENE CARBONATE ; DIMETHYL CARBONATE ; 1,2-PROPYLENE GLYCOL ; AL OXIDE ; CO2 ; CYCLOADDITION ; DIOXIDE ; GLYCEROL ; TRANSESTERIFICATION
WOS研究方向Chemistry ; Physics
语种英语
出版者ELSEVIER
WOS记录号WOS:000568693000016
资助机构Innovation Academy for Green Manufacture, Chinese Academy of Sciences ; "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences ; National Natural Science Foundation of China
内容类型期刊论文
源URL[http://ir.ipe.ac.cn/handle/122111/42067]  
专题中国科学院过程工程研究所
通讯作者Li, Zengxi; Cheng, Weiguo
作者单位1.Dalian Polytech Univ, Sch Light Ind Chem Engn, Dalian 116034, Peoples R China
2.Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China
3.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquids Clean Proc,State Key, Beijing 100190, Peoples R China
4.Chinese Acad Sci, Innovat Acad Green Manufacture, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714
Deng, Lili,Sun, Wenzhong,Shi, Zijie,et al. Highly synergistic effect of ionic liquids and Zn-based catalysts for synthesis of cyclic carbonates from urea and diols[J]. JOURNAL OF MOLECULAR LIQUIDS,2020,316:12.
APA Deng, Lili.,Sun, Wenzhong.,Shi, Zijie.,Qian, Wei.,Su, Qian.,...&Cheng, Weiguo.(2020).Highly synergistic effect of ionic liquids and Zn-based catalysts for synthesis of cyclic carbonates from urea and diols.JOURNAL OF MOLECULAR LIQUIDS,316,12.
MLA Deng, Lili,et al."Highly synergistic effect of ionic liquids and Zn-based catalysts for synthesis of cyclic carbonates from urea and diols".JOURNAL OF MOLECULAR LIQUIDS 316(2020):12.
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