SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 43 ›› Issue (3): 152-160.DOI: 10.1016/j.cjche.2022.02.014

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Covalent organic frameworks-incorporated thin film composite membranes prepared by interfacial polymerization for efficient CO2 separation

Haoqing Xu1,2, Wenyan Feng1,2, Menglong Sheng1,2, Ye Yuan1,2, Bo Wang3, Jixiao Wang1,2, Zhi Wang1,2   

  1. 1. Chemical Engineering Research Center, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China;
    2. Tianjin Key Laboratory of Membrane Science and Desalination Technology, State Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin 300350, China;
    3. Life and Health Research Institute, School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China
  • Received:2021-08-23 Revised:2022-02-21 Online:2022-04-28 Published:2022-03-28
  • Contact: Zhi Wang,E-mail:wangzhi@tju.edu.cn
  • Supported by:
    This research is supported by the National Key Research & Development Program of China (2017YFB0603400), the National Natural Science Foundation of China (21938007).

Covalent organic frameworks-incorporated thin film composite membranes prepared by interfacial polymerization for efficient CO2 separation

Haoqing Xu1,2, Wenyan Feng1,2, Menglong Sheng1,2, Ye Yuan1,2, Bo Wang3, Jixiao Wang1,2, Zhi Wang1,2   

  1. 1. Chemical Engineering Research Center, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China;
    2. Tianjin Key Laboratory of Membrane Science and Desalination Technology, State Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering, Tianjin University, Tianjin 300350, China;
    3. Life and Health Research Institute, School of Chemistry and Chemical Engineering, Tianjin University of Technology, Tianjin 300384, China
  • 通讯作者: Zhi Wang,E-mail:wangzhi@tju.edu.cn
  • 基金资助:
    This research is supported by the National Key Research & Development Program of China (2017YFB0603400), the National Natural Science Foundation of China (21938007).

Abstract: Thin film composite (TFC) membranes with nanofillers additives for CO2 separation show promising applications in energy and environment-related fields. However, the poor compatibility between nanofillers and polymers in TFC membranes is the main problem. In this work, covalent organic frameworks (COFs, TpPa-1) with rich —NH— groups were incorporated into polyamide (PA) segment via in situ interfacial polymerization to prepare defect-free TFC membranes for CO2/N2 separation. The formed covalent bonds between TpPa-1 and PA strengthen the interaction between nanofillers and polymers, thereby enhancing compatibility. Besides, the incorporated COFs disturb the rigid structure of the PA layer, and provide fast CO2 transfer channels. The incorporated COFs also increase the content of effective carriers, which enhances the CO2 facilitated transport. Consequently, in CO2/N2 mixed gas separation test, the optimal TFC (TpPa0.025-PIP-TMC/mPSf) membrane exhibits high CO2 permeance of 854 GPU and high CO2/N2 selectivity of 148 at 0.15 MPa, CO2 permeance of 456 GPU (gas permeation unit) and CO2/N2 selectivity of 92 at 0.5 MPa. In addition, the TpPa0.025-PIP-TMC/mPSf membrane also achieves high permselectivty in CO2/CH4 mixed gas separation test. Finally, the optimal TFC membrane showes good stability in the simulated flue gas test, revealing the application potential for CO2 capture from flue gas.

Key words: Covalent organic frameworks, CO2/N2 separation, In situ interfacial polymerization, Compatibility, Covalent bonds

摘要: Thin film composite (TFC) membranes with nanofillers additives for CO2 separation show promising applications in energy and environment-related fields. However, the poor compatibility between nanofillers and polymers in TFC membranes is the main problem. In this work, covalent organic frameworks (COFs, TpPa-1) with rich —NH— groups were incorporated into polyamide (PA) segment via in situ interfacial polymerization to prepare defect-free TFC membranes for CO2/N2 separation. The formed covalent bonds between TpPa-1 and PA strengthen the interaction between nanofillers and polymers, thereby enhancing compatibility. Besides, the incorporated COFs disturb the rigid structure of the PA layer, and provide fast CO2 transfer channels. The incorporated COFs also increase the content of effective carriers, which enhances the CO2 facilitated transport. Consequently, in CO2/N2 mixed gas separation test, the optimal TFC (TpPa0.025-PIP-TMC/mPSf) membrane exhibits high CO2 permeance of 854 GPU and high CO2/N2 selectivity of 148 at 0.15 MPa, CO2 permeance of 456 GPU (gas permeation unit) and CO2/N2 selectivity of 92 at 0.5 MPa. In addition, the TpPa0.025-PIP-TMC/mPSf membrane also achieves high permselectivty in CO2/CH4 mixed gas separation test. Finally, the optimal TFC membrane showes good stability in the simulated flue gas test, revealing the application potential for CO2 capture from flue gas.

关键词: Covalent organic frameworks, CO2/N2 separation, In situ interfacial polymerization, Compatibility, Covalent bonds