Novel mixed matrix composite membranes containing MCM-41 for CO2 separation

doi:10.11949/j.issn.0438-1157.20150257

Abstract

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 m_MCM-NH2/m_PVAm 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.

Key words: mix matrix membranes, composite membranes, molecular sieves, MCM-41, flue gas, CO₂ capture

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m_MCM-NH2/m_PVAm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。

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

CLC Number:

TQ028.8

HE Yupeng, WANG Zhi, QIAO Zhihua, YUAN Shuangjie, WANG Jixiao. Novel mixed matrix composite membranes containing MCM-41 for CO₂ separation[J]. CIESC Journal, 2015, 66(10): 3979-3990.

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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Novel mixed matrix composite membranes containing MCM-41 for CO₂ separation

含有MCM-41分子筛的混合基质复合膜用于CO₂分离

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