聚乙烯基胺/聚乙烯醇/碳纳米管杂化膜的制备及气体分离性能 |
作者:吴东云,伊春海,鲁妮妮,杨伯伦 |
单位: (西安交通大学,化学工程与技术学院,陕西省能源化工过程强化重点实验室,西安,710049) |
关键词: 聚乙烯基胺/聚乙烯醇聚合物;碳纳米管;有机-无机杂化膜;CO2分离 |
DOI号: |
分类号: TQ028.8 |
出版年,卷(期):页码: 2017,37(2):53-59 |
摘要: |
以聚砜(PS)超滤膜为支撑层,首先制备聚乙烯基胺/聚乙烯醇复合膜,考察PVAm与PVA的组成及铸膜液固含量对膜渗透选择性能的影响。当PVAm/PVA为7/3,固含量为8wt%时,复合膜的性能最好,0.2 MPa下,CO2渗透速率为35.5 GPU(1 GPU=1*10-6 cm3 (STP) cm-2 s-1cmHg-1),CO2/N2的分离系数为123.6。其次,在上述最佳条件中添加不同类型的多壁碳纳米管(MWCNT、MWCNT-OH和MWCNT-COOH),考察碳纳米管含量及表面基团对气体分离性能的影响,并利用红外分析、X-射线衍射及扫描电镜考察所制备杂化膜的化学结构、结晶性能。结果表明,添加表面-OH和-COOH改性的MWCNT可以有效提高膜的透过分离性能。当MWCNT-OH和MWCNT-COOH添加量均为1wt%时,CO2渗透速率分别为62.0和76.6 GPU,CO2/N2的分离系数分别为117.7和139.5。最后,考察进料气压力对杂化膜CO2渗透速率及CO2/N2的分离系数的影响,在0.2~1.8 MPa的压力范围,添加表面改性的碳纳米管均能使复合膜的CO2渗透速率提高。 |
In this paper, the polyvinyl amine (PVAm)/polyvinyl alcohol (PVA) composite membrane was prepared by physical mixing and solution casting on a polysulfone (PSf) support membrane. The effects of the ratio of PVAm to PVA and the casting solution concentration on permselectivity were studied. When the ratio of PVAm and PVA was 7/3 and concentration of casting solution was 8wt%, the composite membrane possessed CO2 permeance of 35.5GPU (1 GPU=1*10-6 cm3 (STP) cm-2 s-1cmHg-1 ) and CO2/N2 selectivity of 123.6 under the condition of 0.2 MPa. Doping different types of multiwall carbon nanotube (MWCNT) under the above optimal condition, the influences of MWCNT content and surface group were investigated. The chemical construction and crystallization property of mixed matrix membrane were characterized by IR, XRD and SEM. The gas permselectivity testing results indicated that the membrane performance can be improved availably by adding MWCNT modified with -OH and -COOH. While the amount of both MWCNT-OH and MWCNT-COOH are 1wt%, the CO2 permeances can reach 62.0GPU and 76.6GPU, and CO2/N2 selectivity are 117.7 and 139.5, respectively. Finally, the impacts of feed pressure on CO2 permeance and CO2/N2 selectivity were explored. It was found that the CO2 permeance increased obviously with adding the MWCNT-OH and MWCNT-COOH when the pressure ranged from 0.2MPa to 1.8MPa. |
基金项目: |
国家自然科学基金(21576217);中央高校基本科研业务费(xjj2016044) |
作者简介: |
作者简介:吴东云(1989-),女,陕西咸阳市人,博士研究生,主要从事气体膜分离研究. 通讯联系人,E-mail:chyi@mail.xjtu.edu.cn |
参考文献: |
[1]Adewole J K, Ahmad A L, Ismail S, et al. Current challenges in membrane separation of CO2 from natural gas: A review[J]. Int J Greenhouse Gas Control, 2013, 17: 46-65. [2]Matteucci S, Kusuma V A, Kelman S D, et al. Gas transport properties of MgO filled poly (1-trimethylsilyl-1-propyne) nanocomposites[J]. Polymer, 2008,49: 1659-1675. [3]Kim S, Marand E. High permeability nano-composite membranes based on mesoporous MCM-41 nanoparticles in a polysulfone matrix[J]. Micropor Mesopor Mater, 2008, 114 : 129-136. [4]Lua A C, Shen Y. Influence of inorganic fillers on the structural and transport properties of mixed matrix membranes[J]. J Appl Polym Sci, 2013, 128: 4058-4066. [5]Zhang Y, Balkus K J, Musselman I H, et al. Mixed-matrix membranes composed of Matrimids and mesoporous ZSM-5 nanoparticles[J]. J Membr Sci, 2008, 325: 28-39. [6]Merkel T C, Freeman B D, Spontak R J, et al. Ultrapermeable, reverse-selective nanocomposite membranes[J]. Science, 2002, 296: 519-522. [7]Vu D Q, Koros W J, Miller S J. Mixed matrix membranes using carbon molecular sieves I. Preparation and experimental results[J]. J Membr Sci, 2003, 211: 311-334. [8]Rajabi Z, Moghadassi A R, Hosseini S M, et al. Preparation and characterization of polyvinylchloride based mixed matrix membrane filled with multi walled carbon nano tubes for carbon dioxide separation[J]. J Ind Eng Chem, 2013, 19: 347-352. [9]Kim S, Chen L, Johnson J K, et al. Polysulfone and functionalized carbon nanotube mixed matrix membranes for gas separation: theory and experiment[J]. J Membr Sci, 2007, 294: 147-158. [10]Aroon M A, Ismail A F, Matsuura T. Beta-cyclodextrin functionalized MWCNT: a potential nano-membrane material for mixed matrix gas separation membranes development[J]. Sep Purif Technol, 2013,115: 39-50. [11]Ahmad A L, Jawad Z A, Low S C, et al. A cellulose acetate/multiwalled carbon nanotube mixed matrix membrane for CO2/N2 separation[J]. J Membr Sci, 2014, 451: 55-66. [12]高翔宇, 贺高红, 梁健. 多壁碳纳米管(MWNT)原丙烯腈(PAN)共混复合膜的制备及性能研究[J]. 膜科学与技术, 2013, 33(3): 17-22 [13]Salih A A M, Yi Chunhai, Peng Hailing, et al. Interfacially polymerized polyetheramine thin film composite membranes with PDMS inter-layer for CO2 separation[J]. J Membr Sci, 2014, 472: 110-118. [14]Furukawa H, Gandara F, Zhang Y B, et al. Water Adsorption in Porous Metal−Organic Frameworks and Related Materials[J]. J Am Chem Soc, 2014, 136: 4369-4381. [15]Amirilargani M, Sadatnia B. Poly(vinyl alcohol)/zeolitic imidazolate frameworks (ZIF-8) mixed matrix membranes for pervaporation dehydration of isopropanol[J]. J Membr Sci, 2014, 469: 1-10. [16]刘迪, 任吉中, 邓麦村. 聚醚共聚酰胺复合气体分离膜的制备与分离性能[J]. 膜科学与技术, 2010, 30(3): 44-49. [17]Cai Y, Wang Z, Yi C H, et al. Gas transport property of polyallylamine-poly(vinyl alcohol)/polysulfone composite membranes[J]. J Membr Sci, 2008, 310: 184-196. |
服务与反馈: |
【文章下载】【加入收藏】 |
《膜科学与技术》编辑部 地址:北京市朝阳区北三环东路19号蓝星大厦 邮政编码:100029 电话:010-64426130/64433466 传真:010-80485372邮箱:mkxyjs@163.com
京公网安备11011302000819号