| 含有MCM-41分子筛的混合基质复合膜用于CO2分离 |
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| 引用本文： | 何玉鹏,王志,乔志华,远双杰,王纪孝.含有MCM-41分子筛的混合基质复合膜用于CO2分离[J].化工学报,2015,66(10):3979-3990. |
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| 作者姓名： | 何玉鹏 王志 乔志华 远双杰 王纪孝 |
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| 作者单位： | 1.天津大学化工学院化学工程研究所, 天津化学化工协同创新中心, 化学工程联合国家重点实验室天津大学, 天津市膜科学与海水淡化技术重点实验室, 天津 300072;2.中国石油天然气管道工程有限公司, 河北 廊坊 065000 |
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| 基金项目： | 国家自然科学基金项目(21436009);国家高技术研究发展计划项目(2012AA03A611)。 |
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| 摘 要： | 为了提高CO2分离膜的性能,将接枝了氨基的MCM-41分子筛(MCM-NH2)添加到聚乙烯基胺(PVAm)水溶液中配制涂膜液,并将PVAm-MCM-NH2涂膜液涂覆到聚砜(PSf)超滤膜上制备PVAm-MCM-NH2/PSf混合基质复合膜。复合膜分离层较薄,有利于CO2渗透速率的提高。接枝的胺基提高了分子筛与聚合物的相容性和膜内胺基含量,有利于膜渗透选择性能的提高。使用CO2/N2混合气(15% CO2 + 85% N2,体积分数)考察了不同MCM-NH2添加量的PVAm-MCM-NH2/PSf膜的渗透选择性能。当涂膜液中mMCM-NH2/mPVAm为0.2、湿涂层厚度为50 μm,测试温度为22℃ 、进料气压力为0.11 MPa时,膜的CO2渗透速率可达4.66×10-7 mol·m-2·s-1·Pa-1,CO2/N2分离因子可达150。较高的CO2/N2分离性能表明PVAm-MCM-NH2/PSf膜在烟道气碳捕集领域具有良好的应用前景。此外,考察了湿涂层厚度、热处理、添加小分子胺等条件对膜渗透选择性能的影响。
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| 关 键 词： | 混合基质膜 复合膜 分子筛 MCM-41 烟道气 二氧化碳捕集 |
| 收稿时间： | 2015-03-03 |
| 修稿时间： | 2015-04-27 |
Novel mixed matrix composite membranes containing MCM-41 for CO2 separation |
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| HE Yupeng,WANG Zhi,QIAO Zhihua,YUAN Shuangjie,WANG Jixiao.Novel mixed matrix composite membranes containing MCM-41 for CO2 separation[J].Journal of Chemical Industry and Engineering(China),2015,66(10):3979-3990. |
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| Authors: | HE Yupeng WANG Zhi QIAO Zhihua YUAN Shuangjie WANG Jixiao |
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| Affiliation: | 1.Chemical Engineering Research Center, School of Chemical Engineering and Technology, Tianjin University, Tianjin Key Laboratory of Membrane Science and Desalination Technology, State Key Laboratory of Chemical Engineering, Collaborative Innovation Center of Chemical Science and Engineering Tianjin, Tianjin 300072, China;2.China Petroleum Pipeline Engineering Corporation, Langfang 065000, Hebei, China |
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| Abstract: | To improve the performance of CO2 separation membrane, MCM-41 modified by amines (MCM-NH2) was filled into polyvinylamine (PVAm) aqueous solution to fabricate PVAm-MCM-NH2 coating solutions. PVAm-MCM-NH2/polysulfone (PSf) mixed matrix composite membranes were prepared by coating PVAm-MCM-NH2 solutions on PSf ultrafiltration membranes. The separation layer of the composite membrane was very thin, which benefited the improvement of CO2 permeance. The amine groups grafted to MCM-41 facilitated the transport of CO2 through reversible reaction and simultaneously improved the filler-polymer interface compatibility. The separation performance of PVAm-MCM-NH2/PSf membranes with different MCM-NH2 content was tested using CO2/N2 mixed gas (15% (vol) CO2 + 85%(vol) N2). When mMCM-NH2/mPVAm in the coating solution was 0.2 at testing temperature of 22℃ and feed gas pressure of 0.11 MPa, the composite membrane exhibited a CO2 permeance of 4.66×10-7 mol·m-2·s-1·Pa-1 and a CO2/N2 selectivity of 150. The high-performance PVAm-MCM-NH2/PSf membrane showed promising applications in CO2 capture from flue gas. Moreover, the effects of the wet coating thickness, the heat treatment and the introduction of the small molecule amines on the separation performance of PVAm-MCM-NH2/PSf membrane were investigated. The results indicated that the increase of wet coating thickness (from 50 μm to 100 μm) with heat treatment under 80℃ or the introduction of ethanediamine would lead to the improvement of the pressure stability, but the loss of CO2/N2 separation performance under low pressures. |
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| Keywords: | mix matrix membranes composite membranes molecular sieves MCM-41 flue gas CO2 capture |
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