无机材料学报 ›› 2012, Vol. 27 ›› Issue (9): 923-927.DOI: 10.3724/SP.J.1077.2012.11655

• 研究论文 • 上一篇    下一篇

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

宋成文1, 姜大伟2, 李 琳2, 孙美悦2, 王同华2   

  1. (1. 大连海事大学 环境科学与工程学院, 大连116026; 2. 大连理工大学 化工学院, 精细化工国家重点实验室炭素研究室, 大连116012)
  • 收稿日期:2011-10-20 修回日期:2011-12-22 出版日期:2012-09-20 网络出版日期:2012-08-28
  • 作者简介:宋成文(1975-), 男, 副教授. E-mail: songchengwen_dmu@yahoo.com.cn
  • 基金资助:

    国家自然科学基金(20776024, 20836006, 20976021); 国家863项目(2009AA03Z215); 辽宁省教育厅高等学校科研计划项目(2009A098); 中央高校基本科研业务费专项基金(2011QN141); 辽宁省海洋与渔业厅海洋环保专题基金(2012-Inhyhbc-0004, 2012-Inhyhbc-0005)

Preparation and Gas Separation Properties of Carbon/Carbon Nanotubes Hybrid Membranes Derived from PMDA-ODA Polyimide

SONG Cheng-Wen1, JIANG Da-Wei2, LI Lin2, SUN Mei-Yue2, WANG Tong-Hua2   

  1. (1. School of Environment Science and Engineering, Dalian Maritime University, Dalian 116026, China; 2. Carbon Research Laboratory and State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116012, China)
  • Received:2011-10-20 Revised:2011-12-22 Published:2012-09-20 Online:2012-08-28
  • About author:SONG Cheng-Wen.E-mail: songchengwen_dmu@yahoo.com.cn
  • Supported by:

    National Natural Science Foundation of China (20776024, 20836006, 20976021); National High-tech Research and Development Project of China (2009AA03Z215); Scientific Research Fund of Liaoning Provincial Education Department (2009A098); Fundamental Research Funds for the Central Universities (2011QN141); Special Foundation for Ocean Environmental Protection of Ocean and Fisheries Department of Liaoning Province (2012-Inhyhbc-0004, 2012-Inhyhbc-0005)

摘要: 针对现有气体分离炭膜存在的渗透速率低等问题, 提出并设计在PMDA-ODA型聚酰亚胺前驱体中掺杂碳纳米管, 经高温热解后制备炭/碳纳米管杂化膜. 分别采用透射电镜(TEM)、X射线衍射分析(XRD)和气体渗透实验对炭/碳纳米管杂化膜的微观结构和分离性能进行表征. 实验结果表明, 在PMDA-ODA型聚酰亚胺前驱体中掺杂碳纳米管后, 碳纳米管与炭基体之间形成明显的“界面间隙”, 打破了原有炭膜中由乱层炭构成的无序微孔结构, 重新构建了杂化炭膜的孔隙结构. 与纯炭膜相比, 杂化炭膜的气体渗透速率大幅增加, 其中O2的渗透速率增大接近4倍(达到1576 Barrer), 而O2/N2的分离选择性仅降低17%.

关键词: 碳纳米管, 聚酰亚胺, 制备, 气体分离

Abstract: A convenient and effective strategy was used to develop a novel carbon/carbon nanotubes (C/CNT) hybrid membrane by incorporating multi-walled carbon nanotubes (MWNT) into PMDA-ODA polyimide precursor through controlled pyrolysis process at 600℃. Transmission electron microscope, X-ray diffraction and gas permeation experiments were employed to investigate the microstructural characteristics and gas separation performance of hybrid carbon membrane. Results show that the as-prepared C/CNT hybrid membrane has excellent gas (H2, CO2, O2, N2 and CH4) separation properties as compared with pure carbon membrane, and the O2 permeability of hybrid carbon membrane increases by nearly 4 times reaching 1576 Barrer, while the O2/N2 permselectivity decreasing by only 17%. It is believed that carbon membrane doped by MWNT can make effective use of the interfacial gaps formed between MWNT and carbon matrix to reconstruct the pore structure of hybrid carbon membrane, which helps to increase the gas diffusion ability and further improve the gas permeability of hybrid carbon membrane.

Key words: carbon nanotubes, polyimide, preparation, gas separation

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