| 聚乙烯胺/Cu3（BTC）2-MMT-NH2混合基质膜的制备及气体传递性能 |
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| 引用本文： | 王立维,王娟娟,王永洪,张新儒,李晋平.聚乙烯胺/Cu3（BTC）2-MMT-NH2混合基质膜的制备及气体传递性能[J].化工学报,2022,73(7):3068-3077. |
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| 作者姓名： | 王立维 王娟娟 王永洪 张新儒 李晋平 |
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| 作者单位： | 1.太原理工大学化学工程与技术学院，山西 太原 030024;2.气体能源高效清洁利用山西省重点实验室，山西 太原 030024 |
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| 基金项目： | 国家自然科学基金面上项目(22078216);山西省回国留学人员科研资助项目(2021-056);山西省自然科学基金面上项目(20210302123196) |
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| 摘 要： | 采用阳离子交换与Cu3(BTC)2原位合成相结合制备Cu3(BTC)2-MMT，同时，借助3-氨基丙基三乙氧基硅烷(KH550)氨基功能化制备Cu3(BTC)2-MMT-NH2杂化材料。然后，将杂化材料添加到聚乙烯胺(PVAm)基质中作为选择性涂层涂覆到聚砜(PSf)支撑体上，制备了PVAm/Cu3(BTC)2-MMT-NH2混合基质膜。通过XRD和FTIR对杂化材料的晶态结构和化学结构进行了表征，同时采用ATR-FTIR证实了Cu3(BTC)2-MMT-NH2杂化材料与PVAm基质之间存在氢键相互作用。系统性研究了PVAm/Cu3(BTC)2-MMT-NH2混合基质膜中MMT阳离子交换量、Cu3(BTC)2-MMT与KH550的质量比、Cu3(BTC)2-MMT-NH2的负载量、操作压力、湿膜厚度、操作温度以及混合气作为原料气对膜CO2渗透性、CO2/N2选择性的影响。结果表明：在纯气气氛，操作温度为25℃、操作压力为1 bar(1 bar=0.1 MPa)的条件下，当Cu3(BTC)2-MMT-NH2负载量为3%(质量)时，膜的气体分离性能最优，CO2渗透率为203 GPU(1GPU=10-6 cm3·cm-2·s-1·cmHg-1，1 cmHg=1333.22 Pa)，CO2/N2选择性为100.7，远高于添加MMT、Cu3(BTC)2和MMT/Cu3(BTC)2混合物的混合基质膜。这是由于Cu3(BTC)2-MMT-NH2具有层间快速传递通道且与聚合物基质有良好的相容性。此外，混合气测试条件下，混合基质膜运行360 h，仍能保持优异的CO2分离性能稳定性。
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| 关 键 词： | 聚乙烯胺 混合基质膜 蒙脱土 传递通道 CO2分离 |
| 收稿时间： | 2022-03-31 |
Gas transport properties of PVAm-based mixed matrix membranes by incorporating with Cu3(BTC)2-MMT-NH2 |
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| Liwei WANG,Juanjuan WANG,Yonghong WANG,Xinru ZHANG,Jinping LI.Gas transport properties of PVAm-based mixed matrix membranes by incorporating with Cu3(BTC)2-MMT-NH2[J].Journal of Chemical Industry and Engineering(China),2022,73(7):3068-3077. |
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| Authors: | Liwei WANG Juanjuan WANG Yonghong WANG Xinru ZHANG Jinping LI |
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| Affiliation: | 1.College of Chemical Engineering and Technology, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China;2.Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization, Taiyuan 030024, Shanxi, China |
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| Abstract: | In this paper, Cu3(BTC)2-MMT was prepared by combining cation exchange with in situ synthesis of Cu3(BTC)2, while Cu3(BTC)2-MMT-NH2 hybrid materials were prepared by amino functionalization of 3-aminopropyltriethoxysilane (KH550). Hybrid materials were added to polyvinylamine (PVAm) matrix as selective coating solution, which was coated on polysulfone (PSf) support to obtain mixed matrix membrane (PVAm/Cu3(BTC)2-MMT-NH2). The crystalline and chemical structures of the hybrid materials were characterized by XRD and FTIR, and hydrogen bonding between the Cu3(BTC)2-MMT-NH2 hybrid materials and the PVAm matrix was confirmed using ATR-FTIR. The effects of exchange of copper and sodium ions, mass ratio of Cu3(BTC)2-MMT to KH550, loading of Cu3(BTC)2-MMT-NH2, operating pressure, wet membrane thickness, operating temperature, and under mixed gas feed on membrane CO2 permeability and CO2/N2 selectivity in mixed matrix membranes were systematically investigated. The results show that under the conditions of pure gas atmosphere, operating temperature of 25℃ and operating pressure of 1 bar, the membrane had the best gas separation performance with a CO2 permeation rate of 203 GPU and CO2/N2 selectivity of 100.7, which is much higher than that of the mixed matrix membrane with MMT, Cu3(BTC)2 or the mixture of MMT and Cu3(BTC)2. This is attributed to the interlayer transmission channel of Cu3(BTC)2-MMT-NH2 and its good compatibility with polymer matrix. In addition, under the mixed gas test condition, the mixed matrix membrane can still maintain excellent stability in CO2 separation performance over 360 h. |
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| Keywords: | polyvinylamine mixed matrix membrane montmorillonite transport passway CO2 separation |
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