具有大侧基和不对称结构含氟聚酰胺的制备及其气体分离性能
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桂林理工大学

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国家自然科学基金资助项目(51963007);广西自然科学基金资助项目(2020GXNSFAA159006,2020GXNSFAA159009);桂林市科学研究与技术开发计划(2020010906)


Fluorinated Polyamide Containing Asymmetric and Bulky Structure: Preparation and Gas Separation Performance
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    摘要:

    以新型二胺单体2,6-双(4-氨基苯基)-4-(3-(1,1,2,2-四氟乙氧基)苯基)吡啶和商品化二酸为原料,合成了三种芳香聚酰胺(PA)。通过FT-IR和NMR表征证实了二胺单体和聚合物的化学结构。PAs均具有良好的有机溶解性,在室温下完全溶于NMP、DMF、DMSO等高沸点有机溶剂,且在加热状态下部分溶解于THF、CHCl3等低沸点有机溶剂中;突出的热稳定性,玻璃化转变温度(Tg)均高于217 ℃,在N2氛围下热失重10%的温度均在512 ℃以上;良好的光学性能,截止波长(λcut-off)及80%透过率的波长(λ80%)范围分别在376 ~ 391 nm和449 ~ 481 nm之间。利用分子动力学模拟计算PAs自由体积分数(FFV),阐明了聚合物引入大侧基和不对称结构有效地抑制分子链的紧密堆积,形成气体传输路径。测定PAs薄膜的He、CO2、O2、N2纯气体渗透性,三种薄膜均表现出较好的气体渗透性。与PA-1、 PA-2相比,PA-3的气体分离性能最好,表现出相对高的P (He) = 11.27 barrer、低的P (N2) = 0.3294 barrer气体渗透性,使得PA-3的He/N2选择性提高,即α (He/N2) = 34.21。

    Abstract:

    Three aromatic polyamides (PA) were synthesized from 2, 6-bis (4-aminophenyl)-4-(3-(1,1,2, 2-tetrafluoroethoxy) phenyl) pyridine and commercial diacid. The chemical structures of diamine monomer and polymer were confirmed by FT-IR and NMR. The prepared PAs have good organic solubility, completely soluble in NMP, DMF, DMSO and other high boiling point organic solvents at room temperature, and partially dissolved in THF, CHCl3 and other low boiling point organic solvents at heating state; Outstanding thermal stability, in which glass transition temperature (Tg) is higher than 217 °C, at the temperature of thermal weight loss of 10% in N2 atmosphere is above 512 °C; good optical performance, the cut-off wavelength (λcut-off) and wavelength of 80% transmittance (λ80%) are in the range of 376 ~ 391 nm and 449 ~ 481 nm, respectively. The free volume fractions of PAs were calculated by molecular dynamics simulation, which clarified that the introduction of large side groups and asymmetric structure into the polymer effectively suppressed the close packing of molecular chains and formed the gas transport path. The PA films were measured for He, CO2, O2, N2 pure gas permeability, three films show relatively similar gas permeability. Compared with PA-1, PA-2, PA-3 has the best gas separation performance, showing relatively high P(He) = 11.27 barrer, low P(N2) = 0.3294 barrer gas permeability, which makes the He/N2 selectivity of PA-3 improved, i.e. α(He/N2) = 34.21.

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  • 收稿日期:2022-03-01
  • 最后修改日期:2022-04-27
  • 录用日期:2022-06-19
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