语种选择
- 个人中心
- 退出登录
浏览全部资源
扫码关注微信
- About Journal
- Indexed-in
- Journal Metrics
您当前的位置：
首页 >
文章列表页 >
Performance and micromechanism of CO2/CH4 separation by ionic liquid-supported misaligned COF membranes
| 更新时间：2026-07-15
|
Performance and micromechanism of CO2/CH4 separation by ionic liquid-supported misaligned COF membranes
- CIESC Journal (2026)
- 作者机构：
1.中国科学院过程工程研究所，固态电池及储能过程北京市重点实验室，北京100190
2.惠州市绿色能源与新材料研究院，广东 惠州516081
3.渤海大学数学科学学院，辽宁 锦州121013
4.沈阳化工大学化学工程学院，辽宁 沈阳110142
5.淮安大学化学工程学院，江苏 淮安223003
- 作者简介：
- 基金信息：
DOI：10.11949/0438-1157.20260457
CLC： TQ 028.8Received：01 April 2026，
Revised：2026-07-09，
Accepted：15 July 2026，
- 稿件说明：
移动端阅览
ZHANG Xiaochun, WANG Qixin, WU Ruiyao, et al. Performance and micromechanism of CO2/CH4 separation by ionic liquid-supported misaligned COF membranes[J/OL]. CIESC Journal, 2026. DOI: 10.11949/0438-1157.20260457.
Performance and micromechanism of CO2/CH4 separation by ionic liquid-supported misaligned COF membranes
摘要
COF膜用于气体分离潜力大，但多数孔道尺寸较大，难以分离动力学直径相近的气体。本研究采用分子动力学模拟方法设计了离子液体负载双层错位COF膜分离CO
2
/CH
4
。研究发现在[Bmim
]
[TF
2
N
]
-错位COF膜中，CO
2
渗透率为6.47×10
4
GPU，CO
2
/CH
4
选择性为21.57。通过对比三种不同阴离子（[TF
2
N
]
⁻、[BF
4
]
⁻和[SCN
]
⁻）分离性能，表明[Bmim
]
[TF
2
N
]
-COF膜分离性能最佳。离子液体在COF膜表面分布结果表明，COF错位后孔道面积减小，离子液体分布更均匀，阳离子和阴离子主要平行于COF表面。通过计算体系相互作用能和径向分布函数发现，COF减弱阳离子和阴离子间的相互作用，促进了离子液体层中气体的传输。离子液体和COF对气体亲和性的差异以及孔道尺寸的减小是CO
2
/CH
4
高效分离的主要原因。
Abstract
Covalent organic framework (COF) membranes hold great potential for gas separation. However
most of their pores have large sizes
making it difficult to separate gases with similar kinetic diameters. In this study
molecular dynamics simulations were employed to design an ionic liquid-supported bilayer staggered COF membrane for CO
2
/CH
4
separation. The results show that the [Bmim
]
[TF
2
N
]
-based misaligned COF membrane achieves a CO
2
permeance of 6.47 × 10
4
GPU and a CO
2
/CH
4
selectivity of 21.57. A comparison of three different anions ([TF
2
N
]
-
[BF
4
]
-
and [SCN
]
-
) reveals that the [Bmim
]
[TF
2
N
]
-COF membrane exhibits the best separation performance. Analysis of ionic liquid distribution on the COF surface indicates that the misalignment reduces the pore area
leading to a more uniform distribution of the ionic liquid
with cations and anions predominantly oriented parallel to the COF surface. Calculation of the interaction energy and radial distribution function reveals that the COF weakens the cation-anion interactions
thereby facilitating gas transport within the ionic liquid layer. The combined effects of the differential affinity of the ionic liquid and COF toward gases
along with the reduced pore size
are identified as the key factors contributing to the high separation of CO
2
/CH
4
.
关键词
Keywords
references
Gür T M . Carbon dioxide emissions, capture, storage and utilization: review of materials, processes and technologies [J ] . Progress in Energy and Combustion Science , 2022 , 89 : 100965 .
Zhu Q J , Zeng Y M , Zheng Y . Overview of CO 2 capture and electrolysis technology in molten salts: operational parameters and their effects [J ] . Industrial Chemistry & Materials , 2023 , 1 ( 4 ): 595 - 617 .
张香平 , 曾少娟 , 冯佳奇 , 等 . CO 2 化工:离子微环境调控的CO 2 绿色高效转化 [J ] . 中国科学:化学 , 2020 , 50 ( 2 ): 282 - 298 .
Zhang X P , Zeng S J , Feng J Q , et al . CO 2 chemical engineering: CO 2 green conversion enhanced by ionic liquid microhabitat [J ] . SCIENTIA SINICA Chimica , 2020 , 50 ( 2 ): 282 - 298 .
Sheng M J , Zhang X , Cheng H Y , et al . Multi-criteria computational screening of [BMIM ] [DCA ] @MOF composites for CO 2 capture [J ] . Green Chemical Engineering , 2025 , 6 ( 2 ): 200 - 208 .
Rozas S , Gennari F C , Atilhan M , et al . Theoretical investigation of carbon dioxide adsorption on MgH 2 with a cobalt catalyst [J ] . Industrial Chemistry & Materials , 2024 , 2 ( 4 ): 587 - 599 .
Zhu J Y , Hou J W , Uliana A , et al . The rapid emergence of two-dimensional nanomaterials for high-performance separation membranes [J ] . Journal of Materials Chemistry A , 2018 , 6 ( 9 ): 3773 - 3792 .
Villalobos L F , Vahdat M T , Dakhchoune M , et al . Large-scale synthesis of crystalline g-C 3 N 4 nanosheets and high-temperature H 2 sieving from assembled films [J ] . Science Advances , 2020 , 6 ( 4 ): eaay9851 .
Zhang K Y , Zhou L W , Wang Z C , et al . Molecular insight into CO 2 /N 2 separation using a 2D-COF supported ionic liquid membrane [J ] . Physical Chemistry Chemical Physics , 2022 , 24 ( 38 ): 23690 - 23698 .
Zhang N , Luo Y , Li Z W , et al . Molecular investigation on the mechanism of permselective transport of CO 2 /N 2 mixture through graphene slit [J ] . Separation and Purification Technology , 2022 , 282 : 119986 .
Qi C X , Song Z , Cheng H Y , et al . A systematic COSMO-RS study on mutual solubility of ionic liquids and C6-hydrocarbons [J ] . Green Chemical Engineering , 2024 , 5 ( 1 ): 97 - 107 .
Xu P , Zhang X C , Zhao L L , et al . Prominently improved CO 2 /N 2 separation efficiency by ultrathin-ionic-liquid-covered MXene membrane [J ] . Separation and Purification Technology , 2023 , 311 : 123296 .
Liu H Y , Zeng S C , Li Z Y , et al . Ionic liquid functionalized covalent organic framework membranes for efficient CO 2 /N 2 separation [J ] . Journal of Membrane Science , 2025 , 729 : 124167 .
Yu Y X , Wang Z L , Zhang X C , et al . Insight into properties and structures of ionic liquids by machine learning molecular dynamics simulation [J ] . Green Energy & Environment , 2026 , 11 ( 2 ): 500 - 510 .
刘亚伟 , 张晓春 , 董坤 , 等 . 离子液体的凝聚态化学研究 [J ] . 化学进展 , 2022 , 34 ( 7 ): 1509 – 1523 .
Liu Y W , Zhang X C , Dong K , et al . Research of condensed matter chemistry on ionic liquids [J ] . Progress in Chemistry , 2022 , 34 ( 7 ): 1509 - 1523 .
Wang Z L , Yan F , Bai L , et al . Insight into CO 2 /CH 4 separation performance in ionic liquids/polymer membrane from molecular dynamics simulation [J ] . Journal of Molecular Liquids , 2022 , 357 : 119119 .
Liu Y M , Guo Y D , Wang Z L , et al . Covalent organic frameworks-confined ionic liquids membranes lead to high-efficient CO 2 /N 2 separation [J ] . Separation and Purification Technology , 2025 , 368 : 132933 .
You L L , Guo Y D , He Y J , et al . Molecular level understanding of CO 2 capture in ionic liquid/polyimide composite membrane [J ] . Frontiers of Chemical Science and Engineering , 2022 , 16 ( 2 ): 141 - 151 .
Guo W , Mahurin S M , Unocic R R , et al . Broadening the gas separation utility of monolayer nanoporous graphene membranes by an ionic liquid gating [J ] . Nano Letters , 2020 , 20 ( 11 ): 7995 - 8000 .
Zhao L L , Guo Y D , Liu P , et al . CO 2 /CH 4 separation through monolayer nanoporous graphene oxide supported ionic liquid membrane [J ] . Journal of Molecular Liquids , 2023 , 390 : 123044 .
Cai J B , Lu L H , Zhu J B , et al . Ionic-liquid-gated porous graphene membranes for efficient CO 2 /CH 4 separation [J ] . Journal of Molecular Liquids , 2022 , 358 : 119148 .
Fan H W , Wang H R , Peng M H , et al . Pore-in-pore engineering in a covalent organic framework membrane for gas separation [J ] . ACS Nano , 2023 , 17 ( 8 ): 7584 - 7594 .
Knebel A , Caro J . Metal-organic frameworks and covalent organic frameworks as disruptive membrane materials for energy-efficient gas separation [J ] . Nature Nanotechnology , 2022 , 17 ( 9 ): 911 - 923 .
Ying Y P , Tong M M , Ning S C , et al . Ultrathin two-dimensional membranes assembled by ionic covalent organic nanosheets with reduced apertures for gas separation [J ] . Journal of the American Chemical Society , 2020 , 142 ( 9 ): 4472 - 4480 .
Zhang Y , Zhang Y , Yan Y L , et al . Microenvironment regulation in hydroxyl-functionalized COF membranes for enhanced CO 2 separation [J ] . Journal of Membrane Science , 2026 , 740 : 124965 .
Tong M M , Yang Q Y , Ma Q T , et al . Few-layered ultrathin covalent organic framework membranes for gas separation: a computational study [J ] . Journal of Materials Chemistry A , 2016 , 4 ( 1 ): 124 – 131 .
Wang P Y , Peng Y , Zhu C Y , et al . Single-phase covalent organic framework staggered stacking nanosheet membrane for CO 2 -selective separation [J ] . Angewandte Chemie International Edition , 2021 , 60 ( 35 ): 19047 - 19052 .
Wang Q X , Guo Y D , Long Y , et al . Efficient separation of CO 2 /CH 4 by covering ultrathin ionic liquid film on COF membrane [J ] . Journal of Membrane Science , 2024 , 701 : 122766 .
Ongari D , Yakutovich A V , Talirz L , et al . Building a consistent and reproducible database for adsorption evaluation in covalent-organic frameworks [J ] . ACS Central Science , 2019 , 5 ( 10 ): 1663 - 1675 .
Delley B . An all‐electron numerical method for solving the local density functional for polyatomic molecules [J ] . The Journal of Chemical Physics , 1990 , 92 ( 1 ): 508 - 517 .
Hess B , Kutzner C , van der Spoel D , et al . GROMACS 4: algorithms for highly efficient, load-balanced, and scalable molecular simulation [J ] . Journal of Chemical Theory and Computation , 2008 , 4 ( 3 ): 435 - 447 .
Sobtop , Version 1.0(dev 5 )[EB/OL ] . http://sobereva.com/soft/Sobtop http://sobereva.com/soft/Sobtop .
Liu Z P , Huang S P , Wang W C . A refined force field for molecular simulation of imidazolium-based ionic liquids [J ] . The Journal of Physical Chemistry B , 2004 , 108 ( 34 ): 12978 - 12989 .
Canongia Lopes J N , Pádua A A H . Molecular force field for ionic liquids composed of triflate or bistriflylimide anions [J ] . The Journal of Physical Chemistry B , 2004 , 108 ( 43 ): 16893 - 16898 .
Zhang X C , Jiang K , Liu Z P , et al . Insight into the performance of acid gas in ionic liquids by molecular simulation [J ] . Industrial & Engineering Chemistry Research , 2019 , 58 ( 3 ): 1443 - 1453 .
Yang Q Y , Liu D H , Zhong C L , et al . Development of computational methodologies for metal–organic frameworks and their application in gas separations [J ] . Chemical Reviews , 2013 , 113 ( 10 ): 8261 - 8323 .
Shi W , Maginn E J . Atomistic simulation of the absorption of carbon dioxide and water in the ionic liquid 1-n-Hexyl-3-methylimidazolium Bistrifluoromethylsulfonyl)imide ([hmim ] [Tf 2 N ] [J ] . The Journal of Physical Chemistry B, 2008, 112 ( 7 ): 2045 - 2055 .
Skoulidas A I , Sholl D S . Transport diffusivities of CH 4 , CF 4 , He, Ne, Ar, Xe, and SF 6 in silicalite from atomistic simulations [J ] . The Journal of Physical Chemistry B , 2002 , 106 ( 19 ): 5058 - 5067 .
Martínez L , Andrade R , Birgin E G , et al . PACKMOL: a package for building initial configurations for molecular dynamics simulations [J ] . Journal of Computational Chemistry , 2009 , 30 ( 13 ): 2157 - 2164 .
Willems T F , Rycroft C H , Kazi M , et al . Algorithms and tools for high-throughput geometry-based analysis of crystalline porous materials [J ] . Microporous and Mesoporous Materials , 2012 , 149 ( 1 ): 134 - 141 .
Wu X W , Han X , Liu Y H , et al . Control interlayer stacking and chemical stability of two-dimensional covalent organic frameworks via steric tuning [J ] . Journal of the American Chemical Society , 2018 , 140 ( 47 ): 16124 - 16133 .
Cheng S Q , Sun X , Ran J X , et al . Tuning asymmetric isomers in one-dimensional covalent organic frameworks to enhance oxygen reduction activity [J ] . Angewandte Chemie International Edition , 2025 , 64 ( 52 ): e20336 .
Li X , Qiao J S , Chee S W , et al . Rapid, scalable construction of highly crystalline acylhydrazone two-dimensional covalent organic frameworks via dipole-induced antiparallel stacking [J ] . Journal of the American Chemical Society , 2020 , 142 ( 10 ): 4932 - 4943 .
Lei Z G , Dai C N , Chen B H . Gas solubility in ionic liquids [J ] . Chemical Reviews , 2014 , 114 ( 2 ): 1289 - 1326 .
Tian Z Q , Mahurin S M , Dai S , et al . Ion-gated gas separation through porous graphene [J ] . Nano Letters , 2017 , 17 ( 3 ): 1802 - 1807 .
Wang W S , Hou Q G , Gong K , et al . Ionic liquid gated 2D-CAP membrane for highly efficient CO 2 /N 2 and CO 2 /CH 4 separation [J ] . Applied Surface Science , 2019 , 494 : 477 - 483 .
Xin Y X , Wang C , Wang Y , et al . Encapsulation of an ionic liquid into the nanopores of a 3D covalent organic framework [J ] . RSC Advances , 2017 , 7 ( 3 ): 1697 - 1700 .
王齐鑫 . 共价有机框架支撑离子液体膜分离CO 2 的模型优化及模拟计算 [D ] . 锦州 : 渤海大学 , 2024 .
Wang Q X . Model optimization and simulation of CO 2 separation by COF supported ionic liquid membrane [D ] . Jinzhou : Bohai University , 2024 .
Zeng S J , Zhang X P , Bai L , et al . Ionic-liquid-based CO 2 capture systems: structure, interaction and process [J ] . Chemical Reviews , 2017 , 117 ( 14 ): 9625 - 9673 .
Zhao R , Wu H , Yang L X , et al . Modification of covalent organic frameworks with dual functions ionic liquids for membrane-based biogas upgrading [J ] . Journal of Membrane Science , 2020 , 600 : 117841 .
查看原文
0
Views
0
下载量
0
CSCD
Alert me when the article has been cited
文章被引用时，请邮件提醒。
提交
Tools
Download
- L-PDFDownload
- WORDDownload
- Meta-XMLDownload
Export Citation
- BibTeXDownload
- EndnoteDownload
- RefMan Download
- NoteExpressDownload
- NoteFirstDownload
Share
Share with wechat friends or circle of friends
Add to favorites
Add to my album
Publicity Resources
Related Articles
Functional ionic liquids for carbon dioxide capture and separation
Removal of CO2 from natural gas by 2-methylimidazole/ethylene glycol system at room temperature
Electric field-assisted preparation of aligned MWCNTs/polystyrene composite membranes for enhanced gas separation performance
Research progress of ionic liquids in separation of aromatics/alkanes and olefins/alkanes
Metal-organic framework encapsulating carbon nanotubes for trace CO2 separation
Related Author
Guokai CUI
Shuzhen LYU
Jianji WANG
TONG Xiongshi
PAN Yong
WANG Muyu
SHI Jialiang
CHEN Guangjin
Related Institution
Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, Key Laboratory of Green Chemical Media and Reactions, Ministry of Education, School of Chemistry and Chemical Engineering, Henan Normal University
State Key Laboratory of Heavy Oil Processing, China University of Petroleum
Petro-China Co. Ltd. Dalian Petrochemical Co.
State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University
State Key Laboratory of Heavy Oil Processing, China University of Petroleum
选择翻译语言
- Technical support is provided by Beijing Founder electronics co., LTD 京ICP备12046843号-3
京公网安备11010102001995号 - It is recommended to read the content of this site in Chrome&IE9+. Please switch to extreme mode in browser 360.
- Cookies We use cookies to help provide and enhance our service and tailor content. By continuing, you agree to the use of cookies.
0
Bulk Citation
Export to
BibTeXEndnoteRefManNoteExpressNoteFirst
TOP