高通量二氧化硅复合膜的制备及其渗透汽化性能研究

硅酸盐通报 ›› 2021, Vol. 40 ›› Issue (7): 2388-2395.

高通量二氧化硅复合膜的制备及其渗透汽化性能研究

刘晓宇^1,2, 吴红丹^1,2, 周志辉^1,2, 李胜利^1,2, 邓思浩^1,2

1.武汉科技大学资源与环境工程学院,武汉 430081;
2.武汉科技大学,冶金矿产资源高效利用与造块湖北省重点实验室,武汉 430081

收稿日期:2021-02-07 修回日期:2021-03-10 出版日期:2021-07-15 发布日期:2021-08-04
通讯作者: 周志辉,博士,副教授。E-mail:13871294049@139.com
作者简介:刘晓宇(1996—),女,硕士研究生。主要从事二氧化硅膜材料的研究。E-mail:lxywust@163.com
基金资助:
湖北省自然科学基金(2018CFB373)

Preparation and Pervaporation Performance of High Flux Silica Composite Membranes

LIU Xiaoyu^1,2, WU Hongdan^1,2, ZHOU Zhihui^1,2, LI Shengli^1,2, DENG Sihao^1,2

1. College of Resources and Environmental Engineering, Wuhan University of Science and Technology, Wuhan 430081, China;
2. Hubei Key Laboratory for Efficient Utilization and Agglomeration of Metallurgic Mineral Resources, Wuhan University of Science and Technology, Wuhan 430081, China

Received:2021-02-07 Revised:2021-03-10 Online:2021-07-15 Published:2021-08-04

摘要/Abstract

摘要： 二氧化硅复合膜展现出的耐酸性和稳定性在渗透汽化领域有着广阔的应用前景。本文采用真空抽吸浸渍法制备二氧化硅复合膜的支撑层,得到高通量二氧化硅复合膜。本文对支撑层真空抽吸的最优条件进行探究,并采用扫描电镜对膜层的表面、截面形貌结构进行表征。结果表明,当支撑层溶胶质量浓度为2%,真空抽吸时间为10 s,真空抽吸压力为0.10 MPa时制备出致密的二氧化硅复合膜,其膜层厚度为6~7 μm。将本文制备的二氧化硅复合膜应用于异丙醇水溶液渗透汽化中,该膜显示出优异的分离性能,其中异丙醇的渗透通量为6.42 kg/(m²·h)。

关键词: 二氧化硅, 复合膜, 真空抽吸浸渍法, 渗透汽化, 分离性能

Abstract: The acid resistance and stability exhibited by silicon composite membranes hold great promise for applications in the field of pervaporation. The support layer of the silica composite membranes were prepared by a vacuum suction dipping method to obtain a high flux silica composite membrane. In this paper, the optimal conditions for vacuum suction of the support layer were explored, and the surface and cross-sectional topography of the membranes were characterized by scanning electron microscope. The results show that when the mass concentration of the supporting layer sol is 2%, the vacuum suction time is 10 s, and the vacuum suction pressure is 0.10 MPa, dense silica composite membranes are prepared with the membrane thickness around 6 μm to 7 μm. The silica composite membranes prepared in this paper are applied to the pervaporation of isopropanol aqueous solution and show excellent separation performance, and the permeation flux of isopropanol is 6.42 kg/(m²·h).

Key words: silica, composite membrane, vacuum suction dipping method, pervaporation, separation performance

中图分类号:

TQ028.8

刘晓宇, 吴红丹, 周志辉, 李胜利, 邓思浩. 高通量二氧化硅复合膜的制备及其渗透汽化性能研究[J]. 硅酸盐通报, 2021, 40(7): 2388-2395.

LIU Xiaoyu, WU Hongdan, ZHOU Zhihui, LI Shengli, DENG Sihao. Preparation and Pervaporation Performance of High Flux Silica Composite Membranes[J]. BULLETIN OF THE CHINESE CERAMIC SOCIETY, 2021, 40(7): 2388-2395.

参考文献

[1] SATO K, SUGIMOTO K, NAKANE T. Preparation of higher flux NaA zeolite membrane on asymmetric porous support and permeation behavior at higher temperatures up to 145 ℃ in vapor permeation[J]. Journal of Membrane Science, 2008, 307(2): 181-195.
[2] RONG H Z, WANG G M, YAN J X, et al. Surface-gel-conversion synthesis of submicron-thick MFI zeolite membranes to expedite shape-selective separation of hexane isomers[J]. Science China Materials, 2021, 64(2): 374-382.
[3] SATO K, SUGIMOTO K, NAKANE T. Preparation of higher flux NaA zeolite membrane on asymmetric porous support and permeation behavior at higher temperatures up to 145 ℃ in vapor permeation[J]. Journal of Membrane Science, 2008, 307(2): 181-195.
[4] 徐子雄,周志辉,吴红丹,等.T型分子筛膜的制备及异丙醇脱水应用[J].硅酸盐学报,2019,47(1):77-83.
XU Z X, ZHOU Z H, WU H D, et al. Preparation of T-type zeolite membrane and application on dehydration of isopropanol[J]. Journal of the Chinese Ceramic Society, 2019, 47(1): 77-83 (in Chinese).
[5] HASEGAWA Y, HOTTA H, SATO K, et al. Preparation of novel chabazite (CHA)-type zeolite layer on porous α-Al₂O₃ tube using template-free solution[J]. Journal of Membrane Science, 2010, 347(1/2): 193-196.
[6] YOSHIMUNE M, MIZOGUCHI K, HARAYA K. Alcohol dehydration by pervaporation using a carbon hollow fiber membrane derived from sulfonated poly(phenylene oxide)[J]. Journal of Membrane Science, 2013, 425/426: 149-155.
[7] TANAKA S, YASUDA T, KATAYAMA Y, et al. Pervaporation dehydration performance of microporous carbon membranes prepared from resorcinol/formaldehyde polymer[J]. Journal of Membrane Science, 2011, 379(1/2): 52-59.
[8] KITAO S, ASAEDA M. Separation of organic acid/water mixtures by thin porous silica membrane[J]. Journal of Chemical Engineering of Japan, 1990, 23(3): 367-370.
[9] VAN VEEN H M, VAN DELFT Y C, ENGELEN C W R, et al. Dewatering of organics by pervaporation with silica membranes[J]. Separation and Purification Technology, 2001, 22/23: 361-366.
[10] ASAEDA M, SAKOU Y, YANG J H, et al. Stability and performance of porous silica-zirconia composite membranes for pervaporation of aqueous organic solutions[J]. Journal of Membrane Science, 2002, 209(1): 163-175.
[11] ASAEDA M, ISHIDA M, TASAKA Y. Pervaporation characteristics of silica-zirconia membranes for separation of aqueous organic solutions[J]. Separation Science and Technology, 2005, 40(1/2/3): 239-254.
[12] YANG J H, YOSHIOKA T, TSURU T, et al. Pervaporation characteristics of aqueous-organic solutions with microporous SiO₂-ZrO₂ membranes: experimental study on separation mechanism[J]. Journal of Membrane Science, 2006, 284(1/2): 205-213.
[13] CASTRICUM H L, SAH A, KREITER R, et al. Hydrothermally stable molecular separation membranes from organically linked silica[J]. Journal of Materials Chemistry, 2008, 18(18): 2150-2158.
[14] IMAI H, MORIMOTO H, TOMINAGA A, et al. Structural changes in sol-gel derived SiO₂ and TiO₂ films by exposure to water vapor[J]. Journal of Sol-Gel Science and Technology, 1997, 10(1): 45-54.
[15] NAGASAWA H, MATSUDA N, KANEZASHI M, et al. Pervaporation and vapor permeation characteristics of BTESE-derived organosilica membranes and their long-term stability in a high-water-content IPA/water mixture[J]. Journal of Membrane Science, 2016, 498: 336-344.
[16] IBRAHIM S M, NAGASAWA H, KANEZASHI M, et al. Organosilica bis(triethoxysilyl)ethane (BTESE) membranes for gas permeation (GS) and reverse osmosis (RO): the effect of preparation conditions on structure, and the correlation between gas and liquid permeation properties[J]. Journal of Membrane Science, 2017, 526: 242-251.
[17] ZHENG F T, YAMAMOTO K, KANEZASHI M, et al. Preparation of bridged silica RO membranes from copolymerization of bis(triethoxysilyl)ethene/(hydroxymethyl)triethoxysilane. Effects of ethenylene-bridge enhancing water permeability[J]. Journal of Membrane Science, 2018, 546: 173-178.
[18] Moriyama N, Nagasawa H, Kanezashi M, et al. Bis(triethoxysilyl)ethane (BTESE)-derived silica membranes: pore formation mechanism and gas permeation properties[J]. Journal of Sol-Gel Science and Technology, 2018, 86: 63-72.
[19] GONG G H, WANG J H, NAGASAWA H, et al. Fabrication of a layered hybrid membrane using an organosilica separation layer on a porous polysulfone support, and the application to vapor permeation[J]. Journal of Membrane Science, 2014, 464: 140-148.
[20] GONG G H, WANG J H, NAGASAWA H, et al. Synthesis and characterization of a layered-hybrid membrane consisting of an organosilica separation layer on a polymeric nanofiltration membrane[J]. Journal of Membrane Science, 2014, 472: 19-28.
[21] 吴红丹,刘宏瑞,刘晓宇,等.二氧化硅复合膜的制备及其渗透汽化性能[J].硅酸盐学报,2020,48(4):592-598.
WU H D, LIU H R, LIU X Y, et al. Preparation and pervaporation of silica composite membrane[J]. Journal of the Chinese Ceramic Society, 2020, 48(4): 592-598 (in Chinese).