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Si-MWCNT/聚酰亚胺混合基质膜的制备及其气体分离性能

Preparation and gas separation properties of Si-MWCNT/polyimide mixed matrix membranes

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    摘要

  • 摘要: 多壁碳纳米管(MWCNTs)因其独特的一维结构和高比表面积在气体分离膜领域备受关注，但其与聚合物基体的相容性差及易团聚等问题限制了其在混合基质膜(MMMs)中的应用。本研究通过酸化处理与硅烷偶联剂(APTES)修饰相结合，制备了表面功能化的Si-MWCNTs，并以其为填料，含氟大侧基聚酰亚胺为基体，采用共混法制备了Si-MWCNTs/聚酰亚胺(PI)混合基质膜。通过FTIR、TGA、XRD及气体渗透性等测试手段对填料与膜材料的结构及性能进行了系统研究。结果表明，Si-MWCNTs表面—OH与—NH2官能团有效增强了其与聚酰亚胺的界面相容性，其管状结构为气体分子提供了快速扩散通道，提升膜材料的渗透性。当Si-MWCNTs负载量为2%时，CO2渗透系数提升至35.63 Barrer (1 Barrer = 10−10 cm3(STP)·cm·cm−2·s−1·cmHg−1)，较纯膜提高69%，CO2/N2分离因子达24.83，提升约85%；尤其O2/N2分离性能超过1991年Robeson上限。研究结果表明，Si-MWCNTs通过协同的结构调控与界面优化，有效突破了传统聚合物膜在气体分离中渗透性与选择性的权衡限制，展现出良好的应用潜力。

     

    Abstract: Multi-walled carbon nanotubes (MWCNTs) have attracted much attention in the field of gas separation membranes due to their unique one-dimensional structure and high specific surface area. However, their poor compatibility with polymer matrices and easy agglomeration limit their application in mixed matrix membranes (MMMs). In this study, surface-functionalized Si-MWCNTs were prepared by combining acidification treatment with silane coupling agent (APTES) modification, and Si-MWCNTs/polyimide (PI) MMMs were prepared by blending Si-MWCNTs with fluorinated polyimide. The structure and properties of the filler and membrane materials were systematically studied by means of FTIR, TGA, XRD and gas permeability. The results show that the introduction of —OH and —NH2 functional groups on the surface of Si-MWCNTs effectively enhances its interfacial compatibility with polyimide and avoids disordered agglomeration. Its tubular structure provides a fast diffusion channel for gas molecules and improves the permeability of the membrane material. When the loading amount of Si-MWCNTs was 2%, the CO2 permeability coefficient increased to 35.63 Barrer, which was 69% higher than that of the pure membrane, and the CO2/N2 separation factor reached 24.83, an increase of about 85%; In particular, the O2/N2 separation performance exceeds the 1991 Robeson upper limit. The results show that Si-MWCNTs effectively break through the trade-off between permeability and selectivity of traditional polymer membranes in gas separation by synergistic structural regulation and interface optimization, showing good application potential.

     

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    参考文献(30)

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