PANI-PVAm/PS纳米复合膜的制备及其CO_2/N_2渗透选择性能研究
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摘要
捕集CO_2等酸性气体的膜分离技术研究已经成为关于能源和环境问题的重大课题之一。固定载体膜是一种用于CO_2捕集很有发展前景的气体分离膜。然而，捕集CO_2的固定载体膜尚处于前期开发阶段，还存在着膜材料种类少以及膜结构难以调控而导致膜性能有待提高的问题。本文首次将多种形貌聚苯胺（PANI）纳米粒子与固定载体膜材料聚乙烯胺(PVAm)混合，制备了一系列具有高CO_2/N_2渗透选择性能的新型CO_2分离膜。
采用化学氧化聚合的方法制备出一系列具有不同形貌的盐酸掺杂的聚苯胺纳米粒子，包括聚苯胺纳米纤维，网状聚苯胺纳米纤维，聚苯胺纳米片。利用溶液共混法制备PANI纳米粒子-PVAm/聚砜（PS）复合膜。利用多种测试手段分析了所制膜的结构。使用CO_2/N_2纯气及混合气（体积比20/80）考察了膜的气体渗透性能。结果表明，PANI纳米粒子的加入扰乱了PVAm链段的堆积，从而减小了膜的结晶度，增加了膜的自由体积，由此提高了膜CO_2/N_2的渗透性能；PANI纳米粒子对于CO_2具有很好的渗透性；PANI纳米粒子对N_2的渗透具有阻隔作用，具有高形状比的PANI纳米片具有最好的N_2阻隔作用；PVAm使得PANI纳米粒子脱掺杂，脱掺杂导致PANI纳米粒子自由体积增加，更有利于小分子CO_2的渗透。
考察了不同掺杂剂掺杂的PANI纳米粒子与PVAm混合制备的纳米复合膜CO_2/N_2渗透选择性能，发现采用水合离子半径小的掺杂剂掺杂的PANI纳米粒子与PVAm混合制备的纳米复合膜具有更高的CO_2/N_2选择性。
研究了PANI纳米粒子的掺杂/脱掺杂过程对PANI-PVAm/PS膜的结构和性能的影响。发现通过PANI纳米粒子的掺杂/脱掺杂过程可以实现膜的微观结构的调控，从而提高膜的CO_2/N_2渗透选择性能。
分析表明聚苯胺纳米颗粒-聚乙烯胺/聚砜复合膜具有理想的气体传递特性，这一特性导致该复合膜具有很好的CO_2/N_2渗透选择性能。
CO_2capture is one of the most important subjects about energy and environment.Fixed carrier membrane is a kind of promising gas separation membrane for CO_2capture. However, fixed carrier membrane for CO_2capture is in an early developmentstage, its performance is not very high due to few membrane materials and thedifficulty in structure control of membrane. In this paper, polyaniline (PANI)nanoparticles with various morphologies were added to the fixed carrier membranematerial polyvinylamine (PVAm) and a series of new membranes with remarkablehigh CO_2/N_2permselectivity were developed.
Polyaniline nanofibers, netlike polyaniline nanofibers and polyaniline nanosheetswere prepared by chemical oxidative polymerization. The PANI-PVAm/polysulfone(PS) nanocomposite membranes were prepared by solution blending. Severaltechniques were employed to characterize the structure of the membrane.Thepermselectivity of nanocomposite membranes was investigated by the pure CO_2andN_2gases and gas mixture containing20vol.%CO_2and80vol.%N_2. The resultsdemonstrate that the inclusion of the PANI nanoparticles to PVAm increases the gasCO_2/N_2permeance of the membranes due to chain packing disruption of PVAmthereby decreasing crystallinity of the membrane and increasing free volume of themembrane; PANI nanoparticles have good CO_2permeance; PANI nanoparticles haveN_2barrier property and the PANI nanosheets due to high aspect ratio have the betterN_2barrier property than other PANI nanoparticles; the PANI nanoparticles werededoped by a reaction of PANI nanoparticles with PVAm; the increased free volumeof PANI nanoparticles by the reaction of PANI nanoparticles with PVAm was moreconducive to CO_2permeance through the PANI nanoparticles.
The effect of dopant species of PANI on the performance of the PANI-PVAm/PSnanocomposite membranes was investigated. It was found that dopant with small sizeof hydrated ion was more conducive to CO_2/N_2selectivity.
The effect of doping/dedoping process of PANI nanoparticles on structure andperformance of the nanocomposite membrane was investigated. The resultsdemonstrated that the microstructure of the membrane can be tuned by doping/dedoping process of PANI nanoparticles and thus good CO_2/N_2permselectivity of the nanocomposite membranes was obtained.
The gas transport characteristic in PANI-PVAm/PS membranes was analysed,which indicated that the characteristic is beneficial for improving the CO_2/N_2separation performance of the membranes.
采用化学氧化聚合的方法制备出一系列具有不同形貌的盐酸掺杂的聚苯胺纳米粒子，包括聚苯胺纳米纤维，网状聚苯胺纳米纤维，聚苯胺纳米片。利用溶液共混法制备PANI纳米粒子-PVAm/聚砜（PS）复合膜。利用多种测试手段分析了所制膜的结构。使用CO_2/N_2纯气及混合气（体积比20/80）考察了膜的气体渗透性能。结果表明，PANI纳米粒子的加入扰乱了PVAm链段的堆积，从而减小了膜的结晶度，增加了膜的自由体积，由此提高了膜CO_2/N_2的渗透性能；PANI纳米粒子对于CO_2具有很好的渗透性；PANI纳米粒子对N_2的渗透具有阻隔作用，具有高形状比的PANI纳米片具有最好的N_2阻隔作用；PVAm使得PANI纳米粒子脱掺杂，脱掺杂导致PANI纳米粒子自由体积增加，更有利于小分子CO_2的渗透。
考察了不同掺杂剂掺杂的PANI纳米粒子与PVAm混合制备的纳米复合膜CO_2/N_2渗透选择性能，发现采用水合离子半径小的掺杂剂掺杂的PANI纳米粒子与PVAm混合制备的纳米复合膜具有更高的CO_2/N_2选择性。
研究了PANI纳米粒子的掺杂/脱掺杂过程对PANI-PVAm/PS膜的结构和性能的影响。发现通过PANI纳米粒子的掺杂/脱掺杂过程可以实现膜的微观结构的调控，从而提高膜的CO_2/N_2渗透选择性能。
分析表明聚苯胺纳米颗粒-聚乙烯胺/聚砜复合膜具有理想的气体传递特性，这一特性导致该复合膜具有很好的CO_2/N_2渗透选择性能。
CO_2capture is one of the most important subjects about energy and environment.Fixed carrier membrane is a kind of promising gas separation membrane for CO_2capture. However, fixed carrier membrane for CO_2capture is in an early developmentstage, its performance is not very high due to few membrane materials and thedifficulty in structure control of membrane. In this paper, polyaniline (PANI)nanoparticles with various morphologies were added to the fixed carrier membranematerial polyvinylamine (PVAm) and a series of new membranes with remarkablehigh CO_2/N_2permselectivity were developed.
Polyaniline nanofibers, netlike polyaniline nanofibers and polyaniline nanosheetswere prepared by chemical oxidative polymerization. The PANI-PVAm/polysulfone(PS) nanocomposite membranes were prepared by solution blending. Severaltechniques were employed to characterize the structure of the membrane.Thepermselectivity of nanocomposite membranes was investigated by the pure CO_2andN_2gases and gas mixture containing20vol.%CO_2and80vol.%N_2. The resultsdemonstrate that the inclusion of the PANI nanoparticles to PVAm increases the gasCO_2/N_2permeance of the membranes due to chain packing disruption of PVAmthereby decreasing crystallinity of the membrane and increasing free volume of themembrane; PANI nanoparticles have good CO_2permeance; PANI nanoparticles haveN_2barrier property and the PANI nanosheets due to high aspect ratio have the betterN_2barrier property than other PANI nanoparticles; the PANI nanoparticles werededoped by a reaction of PANI nanoparticles with PVAm; the increased free volumeof PANI nanoparticles by the reaction of PANI nanoparticles with PVAm was moreconducive to CO_2permeance through the PANI nanoparticles.
The effect of dopant species of PANI on the performance of the PANI-PVAm/PSnanocomposite membranes was investigated. It was found that dopant with small sizeof hydrated ion was more conducive to CO_2/N_2selectivity.
The effect of doping/dedoping process of PANI nanoparticles on structure andperformance of the nanocomposite membrane was investigated. The resultsdemonstrated that the microstructure of the membrane can be tuned by doping/dedoping process of PANI nanoparticles and thus good CO_2/N_2permselectivity of the nanocomposite membranes was obtained.
The gas transport characteristic in PANI-PVAm/PS membranes was analysed,which indicated that the characteristic is beneficial for improving the CO_2/N_2separation performance of the membranes.
引文
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