石墨烯/聚酰亚胺炭膜的制备及其气体分离性能

侯旻辰; 李琳; 鲁云华; 冉旭; 宋成文; 王春雷; 梁长海; 王同华

doi:10.19869/j.ncm.1007-8827.20180067

石墨烯/聚酰亚胺炭膜的制备及其气体分离性能

doi: 10.19869/j.ncm.1007-8827.20180067

侯旻辰^1,2,
李琳^2,,
鲁云华³,
冉旭⁴,
宋成文⁵,
王春雷²,
梁长海^1,2,
王同华²

1.
大连理工大学石油与化学工程学院, 辽宁盘锦 124221;
2.
大连理工大学化工学院, 精细化工国家重点实验室, 炭素材料研究所炭膜及多孔炭材料课题组, 辽宁大连 116024;
3.
辽宁科技大学化学工程学院, 辽宁鞍山 114051;
4.
哈尔滨铁路公安局刑事技术处, 黑龙江哈尔滨 150001;
5.
大连海事大学环境科学与工程学院, 辽宁大连 116026

基金项目: 国家重点研发计划（2017YFB0603403）；国家自然科学基金（21476034，21506020，21676044，21576035，21978034）；中央高校基本科研业务费（DUT2018TB02）；大连市科技创新基金（2018J12GX031）.

详细信息

作者简介:
侯旻辰,硕士研究生.E-mail:hmc19921209@163.com

通讯作者:
李琳,副教授.E-mail:lindalee121@126.com;王同华,教授.E-mail:wangth@dlut.edu.cn

中图分类号: TB383
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出版历程
- 收稿日期: 2018-05-17
- 修回日期: 2019-11-06
- 刊出日期: 2020-12-31

The preparation and gas separation performance of graphene/polyimide carbon membranes

1.
School of Petroleum and Chemical Engineering, Dalian University of Technology, Panjin 124221, China;
2.
Groups of Carbon Membrane and Porous Carbon Materials, Carbon Research Laboratory, State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China;
3.
School of Chemical Engineering, University of Science and Technology Liaoning, Anshan 114051, China;
4.
Harbin Railway Public Security Bureau, Harbin 150001, China;
5.
School of Environment Science and Engineering, Dalian Maritime University, Dalian 116026, China

Funds: National Key Research and Development Program of China (2017YFB0603403);National Natural Science Foundation of China (21476034,21506020,21676044,21576035,21978034),Fundamental Research Funds for the Central Universities(DUT2018TB02),Innovation Funds for Dalian Science and Technology(2018J12GX031).

摘要

摘要: 以9，9-双（4-氨基苯基芴）（FDA）、9，9-双（3-氨基-4-羟基苯基）芴（BisAHPF）、六氟二酐（6FDA）为单体，二维片层氧化石墨烯（GO）纳米炭晶为孔尺度调节剂，采用原位合成法制备GO/聚酰亚胺聚合物，经制膜及高温炭化制备了石墨烯/聚酰亚胺气体分离炭膜。借助于FTIR、XPS、XRD、TGA、氮吸附及气体渗透等表征手段对GO及炭膜的结构与性能进行表征；探讨了GO添加量对石墨烯/聚酰亚胺炭膜的结构与性能的影响。结果表明，原位引入片状GO纳米炭晶，在改善了聚合物膜热稳定性的同时，显著提高了石墨烯/聚酰亚胺炭膜的总孔体积，特别是尺度小于0.6 nm的极微孔孔体积与数量；使石墨烯/聚酰亚胺炭膜在保持高气体渗透性条件下，明显地提高气体分离选择性；增加GO添加量，可进一步提升石墨烯/聚酰亚胺炭膜的气体分离选择性。当GO添加量为0.5 wt.%时，石墨烯/聚酰亚胺炭膜的CO₂渗透系数为8 760 Barrer，比纯炭膜仅降低了6%；CO₂/N₂、CO₂/CH₄分离选择性分别为52、53，分别提高32%、39%。
- 氧化石墨烯 /
- 炭膜 /
- 原位聚合 /
- 气体分离
Abstract: Graphene/polyimide carbon membranes were prepared by an in-situ polymerization method, in which the 9,9'-bis(4-aminophenyl)fluorine (FDA), 9,9'-bis(3-amino-4-hydroxyphenyl)fluorine (BisAHPF) and 4,4'- (hexafluoroisopropylidene)diphthalic anhydride (6FDA) were used as the monomers and graphene oxide (GO) as the pore size regulator. FTIR, XPS, XRD, TGA, N₂ adsorption and gas permeability tests were used to characterize the microstructures and properties of GO and the graphene/polyimide carbon membranes. The effect of the GO content on the microstructure and gas separation performance of the carbon membranes were investigated. Results show that the incorporation of GO into the polyimide significantly increases the total pore volume of the carbon membranes, especially the volume of ultramicropores smaller than 0.6 nm, as well as improving the thermal stability of the membranes. Compared with the polyimide carbon membrane without GO, the graphene/polyimide carbon membranes have an obvious increase in the CO₂ selectivity with a high gas permeability and the selectivity increased with GO loading. The gas permeability of pure CO₂ for the graphene/polyimide carbon membrane with a GO loading of 0.5 wt.% is 8 760 Barrer and its CO₂ selectivities against N₂ (CO₂/N₂) and CH₄(CO₂/CH₄) are 52 and 53, respectively, which are 32%, and 39% higher than that of the pure carbon membrane.
- Graphene oxide /
- Carbon membrane /
- in-situ polymerization /
- Gas separation

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参考文献(26)

Kamath M G, Fu S, Itta A K, et al. 6FDA-DETDA:DABE polyimide-derived carbon molecular sieve hollow fiber membranes:Circumventing unusual aging phenomena[J]. Journey of Membrane Science, 2018, 546:197-205.

Koros W J, Fleming G K. Membrane-based gas separation[J]. Journal of Membrane Science, 1993, 83:1-80.

Robeson L M. The upper bound revisited[J]. Journey of Membrane Science, 2008, 320:390-400.

L Li, Wang T H. Preparation and gas separation performance of supported carbon membranes with ordered mesoporous carbon interlayer[J]. Journey of Membrane Science, 2014, 450:469-477.

Carta M, Malpass-Evans R, Croad M, et al. An Efficient polymer molecular sieve for membrane gas separations[J]. Science, 2013, 339(6117):303-307.

Bernardo P, Drioli E, Golemme G. Membrane gas separation:A review/state of the art[J]. Industrial & Engineering Chemistry Research, 2009, 48(10):4638-4663.

Koros W J, Zhang C. Materials for next-generation molecularly selective synthetic membranes[J]. Nature Materials, 2017, 16(3):289.

Li L, Wang T H, Liu Q L, et al. A high CO₂ perrmselective mesoporous silica/carbon composite membrane for CO₂ separation[J]. Carbon, 2012, 50(14):5186-5195.

Fu S, Sanders E S, Koros W J. Temperature dependence of gas transport and sorption in carbon molecular sieve membranes derived from four 6FDA based polyimides:Entropic selectivity evaluation[J]. Carbon, 2015, 95:995-1006.

Rungta M, Wenz G B, Zhang C, et al. Carbon molecular sieve structure development and membrane performance relationships[J]. Carbon, 2017, 115:237-248.

Hamm J B S, Ambrosi A, Griebeler J G, et al. Recent advances in the development of supported carbon membranes for gas separation[J]. International Journal of Hydrogen Energy, 2017, 42:24830-24845.

Fu S, Sanders E S, Kulkarni S S, et al. Carbon molecular sieve membrane structure-property relationships for four novel 6FDA based polyimide precursors[J]. Journal of Membrane Science, 2015, 487:60-73.

宋晶, 李琳, 徐瑞松,等. CO₂捕集炭膜的前驱体结构设计及性能[J]. 高等学校化学学报, 2017, 38(10):1850-1856. (SONG Jing, LI Lin, LU Yunhua, et al. Precursors structural design and property of carbon membrane for CO2 capture[J]. Chemical Journal of Chinese Universities, 2017, 38(10):1850-1856.)

宋成文, 姜大伟, 李琳,等. PMDA-ODA型聚酰亚胺炭/碳纳米管杂化膜的制备及气体分离性能研究[J]. 无机材料学报, 2012, 27(9):923-927. (SONG Cheng-Wen, JIANG Da-Wei, LI Lin, et al. Preparation and Gas Separation Properties of Carbon/Carbon Nanotubes Hybrid Membranes Derived from PMDA-ODA Polyimide[J]. Journal of Inorganic Materials, 2012, 27(9):923-927.)

Moore T T, Mahajan R, Koros W J, et al. Hybrid membrane materials comprising organic polymers with rigid dispersed phases[J].AIChe Journal, 2004, 50:311-321.

赵选英,王同华,曹义鸣,等. Fe/C杂化炭膜的制备及其气体分离性能[J]. 化工学报,2009, 60(9):2233-2235(ZHAO Xuanying,WANG Tonghua,LI Lin,et al. Fabrication of Fe/C hybrid carbon membranes for gas separation[J]. CIESC Journal, 2009, 60(9):2232-2236.)

Li L, Song C W, Jiang D W, et al. Preparation and enhanced gas separation performance of carbon/carbon nanotubes (C/CNTs) hybrid membranes[J]. Separation and Purification Technology, 2017, 188:73-80.

Li L, Wang C L, Wang N, Wang T H, et al. The preparation and gas separation properties of zeolite/carbon hybrid membranes[J]. Journal of Materials Science, 2015, 50(6):2561-2670.

JING Guo-jian, YE Zheng-mao, LI Cheng, et al. A ball milling strategy to disperse graphene oxide in cement composites[J]. New Carbon Materials, 2019, 34(6):569-577.

Dong G Y, Hou J W, Zhang Y T, et al. Enhanced CO₂/N₂ separation by porous reduced graphene oxide/Pebax mixed matrix membranes[J]. Journey of Membrane Science, 2016, 520:860-868.

Shen J, Liu G P, Jin W Q, et al. Membranes with fast and selective gas-transport channels of laminar graphene oxide for efficient CO₂ capture[J], Angewandte Chemie International Edition, 2015, 54:578-582.

Lu Y H, Hao J C, Li L, et al. Preparation and gas transport properties of thermally induced rigid membranes of copolyimide containing cardo moieties[J]. Reactive and Functional Polymers, 2017, 119:134-144.

Hummers W S, Offeman R E. Preparation of graphitic oxide[J]. Journal of the American Chemical Society, 1958, 80(6):1339.

GAO Xiang-li, LIU Cui-xian, HAN Gao-yi, et al. Reduced graphene oxide hydrogels prepared in the presence of phenol for high-performance electrochemical capacitors[J]. New Carbon Materials, 2019, 34(5):403-416.

孙美悦, 李琳, 王同华, 等. P25杂化炭膜的制备及其气体分离性能[J]. 无机材料学报, 2013, 28(5):486-490. (Mei-Yue SUN, Lin LI, Ping-Ping ZHANG, et al. Preparation and gas separation performance of P25 hybrid carbon membranes[J]. Journal of Inorganic Materials, 2013, 28(5):485-489.)

Lu Y, Hao J, Xiao G, et al. Preparation and properties of in situ amino-functionalized graphene oxide/polyimide composite films[J]. Applied Surface Science, 2017, 422:710-719.

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