SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2023, Vol. 55 ›› Issue (3): 202-211.DOI: 10.1016/j.cjche.2022.05.018

• Full Length Article • 上一篇    下一篇

Efficient conversion of CO2 into cyclic carbonates under atmospheric by halogen and metal-free poly(ionic liquid)s

Bowen Jiang, Jia Liu, Guoqiang Yang, Zhibing Zhang   

  1. School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
  • 收稿日期:2022-01-17 修回日期:2022-05-10 出版日期:2023-03-28 发布日期:2023-06-03
  • 通讯作者: Guoqiang Yang,E-mail:ygq@nju.edu.cn;Zhibing Zhang,E-mail:zbzhang@nju.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (21776122, 21676134, 21878141 and 21576129) and Natural Science Foundation of Jiangsu Province (BM2018007, BK20210185).

Efficient conversion of CO2 into cyclic carbonates under atmospheric by halogen and metal-free poly(ionic liquid)s

Bowen Jiang, Jia Liu, Guoqiang Yang, Zhibing Zhang   

  1. School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China
  • Received:2022-01-17 Revised:2022-05-10 Online:2023-03-28 Published:2023-06-03
  • Contact: Guoqiang Yang,E-mail:ygq@nju.edu.cn;Zhibing Zhang,E-mail:zbzhang@nju.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21776122, 21676134, 21878141 and 21576129) and Natural Science Foundation of Jiangsu Province (BM2018007, BK20210185).

摘要: A novel series of halogen free, hydroxyl group containing poly(ionic liquid)s (PILs) was first synthesized from glycerol dimethyl acrylate (GDA) and 1-vinyl imidazole (1-VIM) through free radical polymerization, follow by an alkylation step and an ion-exchange procedure to form the final imidazolium hydrogen carbonate heterogenous catalyst poly(HCO3-OH-n). The chemical and physical properties were investigated by varying the monomer ratio between GDA and 1-VIM. Among them, poly (HCO3-OH-2) exhibited the highest catalytic activity for CO2 cycloaddition, with the yield of chloropropene carbonate 90% under mild conditions (80 ℃, 0.1 MPa, 12 h, 0.15 g catalyst for 32 mmol epichlorohydrin) in the absence of any cocatalyst, metal or solvent. A range of substrates with good to excellent yields under atmosphere was obtained. The poly(HCO3-OH-n) catalyst is collectable and still remains acceptable catalytic activity after six runs. Finally, a preliminary kinetic is calculated on the basis of poly(HCO3-OH-2) with the activation energy value of 79.5 kJ·mol-1. This study highlights that the poly(HCO3-OH-n) enable to reach efficient CO2 conversion under mild conditions.

关键词: Ion exchange, Carbon dioxide, Polymerization, Heterogeneous catalyst, Kinetic modeling

Abstract: A novel series of halogen free, hydroxyl group containing poly(ionic liquid)s (PILs) was first synthesized from glycerol dimethyl acrylate (GDA) and 1-vinyl imidazole (1-VIM) through free radical polymerization, follow by an alkylation step and an ion-exchange procedure to form the final imidazolium hydrogen carbonate heterogenous catalyst poly(HCO3-OH-n). The chemical and physical properties were investigated by varying the monomer ratio between GDA and 1-VIM. Among them, poly (HCO3-OH-2) exhibited the highest catalytic activity for CO2 cycloaddition, with the yield of chloropropene carbonate 90% under mild conditions (80 ℃, 0.1 MPa, 12 h, 0.15 g catalyst for 32 mmol epichlorohydrin) in the absence of any cocatalyst, metal or solvent. A range of substrates with good to excellent yields under atmosphere was obtained. The poly(HCO3-OH-n) catalyst is collectable and still remains acceptable catalytic activity after six runs. Finally, a preliminary kinetic is calculated on the basis of poly(HCO3-OH-2) with the activation energy value of 79.5 kJ·mol-1. This study highlights that the poly(HCO3-OH-n) enable to reach efficient CO2 conversion under mild conditions.

Key words: Ion exchange, Carbon dioxide, Polymerization, Heterogeneous catalyst, Kinetic modeling