SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 42 ›› Issue (2): 170-177.DOI: 10.1016/j.cjche.2021.09.003

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Screening and design of COF-based mixed-matrix membrane for CH4/N2 separation

Tongan Yan1, Dahuan Liu1, Qingyuan Yang1, Chongli Zhong2   

  1. 1. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China;
    2. State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China
  • Received:2021-05-29 Revised:2021-08-27 Online:2022-03-30 Published:2022-02-28
  • Contact: Dahuan Liu,E-mail:liudh@mail.buct.edu.cn;Qingyuan Yang,E-mail:qyyang@mail.buct.edu.cn
  • Supported by:
    This work was financially supported by the National Key Research & Development Program of China (2021YFB3802200) and the National Natural Science Foundation of China (Nos. 22078004 and 21978005).

Screening and design of COF-based mixed-matrix membrane for CH4/N2 separation

Tongan Yan1, Dahuan Liu1, Qingyuan Yang1, Chongli Zhong2   

  1. 1. State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China;
    2. State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China
  • 通讯作者: Dahuan Liu,E-mail:liudh@mail.buct.edu.cn;Qingyuan Yang,E-mail:qyyang@mail.buct.edu.cn
  • 基金资助:
    This work was financially supported by the National Key Research & Development Program of China (2021YFB3802200) and the National Natural Science Foundation of China (Nos. 22078004 and 21978005).

Abstract: Membrane separation is a high-efficiency, energy-saving, and environment-friendly separation technology. Covalent organic framework (COF)-based mixed-matrix membranes (MMMs) have broad application prospects in gas separation and are expected to provide new solutions for coal-bed methane purification. Herein, a high-throughput screening method is used to calculate and evaluate COF-based MMMs for CH4/N2 separation. General design rules are proposed from thermodynamic and kinetic points of view using the computation-ready, experimental COFs. From our database containing 471,671 generated COFs, 5 COF membrane materials were screened with excellent membrane selectivities, which were then used as the filler of MMMs for separation performance evaluation. Among them, BAR-NAP-Benzene_CF3 combined with polydimethylsiloxane and styrene-b-butadiene-b-styrene show high CH4 permeability of 4.43×10-13 mol·m·s-1·Pa-1·m-2 and high CH4/N2 selectivity of 9.54, respectively. The obtained results may provide reasonable information for the design of COF-based membranes for the efficient separation of CH4/N2.

Key words: Covalent organic frameworks, Methane, Molecular simulations, Mixed-matrix membrane, Nitrogen, Separation

摘要: Membrane separation is a high-efficiency, energy-saving, and environment-friendly separation technology. Covalent organic framework (COF)-based mixed-matrix membranes (MMMs) have broad application prospects in gas separation and are expected to provide new solutions for coal-bed methane purification. Herein, a high-throughput screening method is used to calculate and evaluate COF-based MMMs for CH4/N2 separation. General design rules are proposed from thermodynamic and kinetic points of view using the computation-ready, experimental COFs. From our database containing 471,671 generated COFs, 5 COF membrane materials were screened with excellent membrane selectivities, which were then used as the filler of MMMs for separation performance evaluation. Among them, BAR-NAP-Benzene_CF3 combined with polydimethylsiloxane and styrene-b-butadiene-b-styrene show high CH4 permeability of 4.43×10-13 mol·m·s-1·Pa-1·m-2 and high CH4/N2 selectivity of 9.54, respectively. The obtained results may provide reasonable information for the design of COF-based membranes for the efficient separation of CH4/N2.

关键词: Covalent organic frameworks, Methane, Molecular simulations, Mixed-matrix membrane, Nitrogen, Separation