SiO2及Ag+-SiO2填充PEBAX/PAN复合膜渗透汽化分离噻吩
作者:刘琨,韩健健,付夏娜,程静静
单位: 广西大学 广西石化资源加工及过程强化技术重点实验室, 南宁 530004
关键词: 聚醚共聚酰胺(PEBAX);SiO2;膜;渗透汽化;噻吩
DOI号:
分类号: TQ028.8
出版年,卷(期):页码: 2015,35(4):7-12

摘要:
采用经典Stöber方法制备了微米固体SiO2(μ- SiO2)及Ag+修饰SiO2颗粒(Ag+-SiO2)。以纳米气相SiO2(n- SiO2)、μ- SiO2以及Ag+-SiO2为填充物,分别制备了PEBAX/PAN复合膜及三种填充型复合膜。XRD、FTIR分别考察了修饰前后颗粒的晶体结构情况及成分,SEM表征了Ag+-SiO2及膜的形貌结构。另外,还研究考察了膜在噻吩/正庚烷溶液中的溶胀情况,结果显示:随料液噻吩含量的增加溶胀度增大,膜溶胀度大小顺序为:Ag+-SiO2填充型复合膜(PMSA)> n- SiO2填充型复合膜(PMS1)>μ- SiO2填充型复合膜(PMS2)>复合膜(PM)。渗透汽化实验考查了上述四种膜分离噻吩能力,结果表明:三种填充型复合膜分离因子得到提高,但渗透通量有所降低,其中PMSA分离性能最佳。在填充量为5%、温度为30℃,以及料液噻吩含量为1000ppm时,PMSA的分离因子为4.2,渗透通量为2.8kg/m2·h。
 
Silica microspheres and silver/silica core–shell microspheres were prepared by the method of Stöber. Composite membrane of polyether block amide /polyacrylonitrile (PEBAX/PAN) and mixed matrix membranes with nano-fumed silica, silica microspheres and Ag+-SiO2 core–shell microspheres as the filler, were prepared. The formation and composition of the particles before modified and after were characterized by XRD and FTIR, respectively. The structure morphology of Ag+-SiO2 core–shell microspheres and the membranes were respectively characterized by SEM. In addition, swelling situation of membranes was explored. The experimental results display that the swelling degree of the membranes in model gasoline with thiophene and n-heptane increases with thiophene content. The swelling degree of the membranes as follow: Ag+-SiO2 filled membrane(PMSA)> nano-fumed silica filled membrane(PMS1)> silica microspheres(PMS2)> composite membrane(PM). The separation abilities to thiophene of four membranes were systematically investigated by pervaporation experiments. That experimental results showed that separation factor of three filled-composite membranes all was intensified, but their fluxes decreased slightly. It also exhibited the PMSA has the best separation performance, its separation factor and the total flux were 4.2 and 2.8kg·m-2·h-1 respectively, under the thiophene concentration 1000ppm and at 30℃.
 

基金项目:
广西石化资源加工及过程强化技术重点实验室主任基金(2013Z009);广西自然科学基金(2014jjAA20079)

作者简介:
刘琨(1962—),女,广西南宁,博士,教授,广西大学化学化工学院博士生导师,主要从事膜分离研究。

参考文献:
[1]  陈剑,李继定,亓荣彬,等.PEG/PEI复合膜渗透汽化汽油脱硫研究(1)制膜条件影响[J].膜科学与技术,2009, 29(4): 39-43..
[2]  陈天泉,陈金勋,李继定,等.正庚烷/有机硫体系渗透汽化脱硫[J].膜科学与技术,2007, 27(4): 87-90.
[3]  孙志娟,余谟鑫,张心亚,等.油品中噻吩类硫化物脱除技术研究进展[J].化工进展,2005, 24(9): 1002-1005.
[4]  Mortaheb H R, Ghaemmaghami F, Mokhtarani B. A Review on Removal of Sulfur Components from Gasoline by Pervaporation [J]. Chem Eng Res Des, 2012, 90: 409-432.
[5]  林立刚,张玉忠.膜技术在汽油脱硫中应用的新进展[J].石油学报(石油加工),2010,26(3): 476-485.
[6]  孔瑛,张玉忠,林立刚,等.汽油脱硫用复合膜的制备及性能[J].高分子材料科学与工程,2010,26(5): 127-129.
[7]  车竹梅,孙本惠,陈翠仙,等.ZSM一5分子筛填充硅橡胶膜在乙醇/水体系中的溶胀特性[J].膜科学与技术,2009, 29(4): 53-56.
[8]  刘琨,陈松.碳分子筛填充聚醚共聚乙酰胺膜渗透汽化分离水溶液中的醋酸正丁酯[J].膜科学与技术,2010, 30(2): 45-51.
[9]  Cao R J, Zhang X F, Wu H, et al. Enhanced pervaporative desulfurization by polydimethylsiloxane membranesembedded with silver/silica core-shell microspheres[J]. J Hazard Mater, 2011, 187: 324-332.
[10]  Liu W P, Li B, Cao R J, et al. Enhanced pervaporation performance of poly (dimethyl siloxane) membrane by incorporating titania microspheres with high silver ion loading [J]. J Membr Sci, 2011, 378: 382– 392.
[11]  Qi R B, Wang Y J, Chen J, et al. Pervaporative desulfurization of model gasoline with Ag2O-filled PDMS membranes [J]. Sep Purif Technol, 2007, 57: 170–175.
[12]  Qi R B, Wang Y J, Chen J, et al. Removing thiophenes from n-octane using PDMS–AgY zeolite mixed matrix membranes [J]. J Membr Sci, 2007, 295: 114–120.
[13]  Lin L G, Wang A D, Dong M M et al. Sulfur removal from fuel using zeolitespolyimide mixed matrix membrane adsorbents[J]. J Hazard Mater, 2012, 203-204: 204-212.
[14]  陈剑,李继定,亓荣彬,等. PDMS/PEI复合膜对FCC汽脱硫性能(III)Ag2O载体促进传递[J].膜科学与技术,2009, 29(3): 39-44.
[15]  姜小阳,李霞.纳米二氧化硅微球的应用及制备进展[J].硅酸盐通报,2011, 30(3): 577-582.
[16]  Liu K, Tong Z F, Liu L et a1. Separation of Organic Compounds from Water by Pervaporation in The Production of N-n-butyl Acetate via Esterification by Reactive Distillation[J]. J Membr Sci, 2005, 256: 193-201.
[17]  Ahmet E Y, Hilmioglu N D, Tulbentci S. Separation of Benzene/Cyclohexane Mixtures by Pervaporation Using PEBA Membranes [J]. Desalination, 2008, 219: 14-25.
[18]  Liu K, Fang C J, Li Z Q et a1. Separation of thiophene/n-heptane mixtures using PEBAX/PVDF-composited membranes via pervaporation[J]. J Membr Sci, 2014, 451: 24-31.
[19]  Timothy C M, Rolande B, Isabelle C, et a1.Silver salt facilitated transport membranes for olefin/paraffin separations: Carrier instability and a novel regeneration method[J]. J Membr Sci, 2013, 447: 177-189.
[20]  Tan H F, Wu Y H, Zhou Y, et a1. Pervaporative recovery of n-butanol from aqueous solutions with MCM-41 filled PEBA mixed matrix membrane[J]. J Membr Sci, 2014, 453: 202-311.
[21]  邹昀,杨超,刘琨,等.醋酸丁酯酯化反应体系组分在PEBA膜中的吸附性能[J].高校化学工程学报,2009, 23(1): 18-22.
[22]  刘琨,杨超,陈松,等.聚醚共聚酰胺(PEBAX)膜的溶胀和渗透汽化行为研究[J].高校化学工程学报,2010, 24(1): 16-21.
[23]  Werner S, Arthur F. Controlled Growth of Monodisperse Silica Spheres in the Micron Size Range[J]. J Colloid Interf Sci,1968, 26: 62-69.
[24]  Sampranpiboon P R, Jiraratananon D U, Hang R Y M. Pervaporation separation of ethyl butyrate and isopropanol with polyether block amide (PEBAX) membranes [J]. J Membr Sci, 2000, 173: 53-59.
[25]  郭树军,周新木,刘厚凡,等.稻壳制备高纯白炭黑的工艺研究[J].粮油食品科技,2010,18(5):13-16.
[26]  张晓丹,张东辉.介孔二氧化硅负载银离子吸附脱除甲硫醚[J].化工进展,2011,30:268-271.
[27]  陈和生,孙振亚,邵景昌.八种不同来源二氧化硅的红外光谱特征研究[J].硅酸盐通报,2011,30(4):934-937.
[28]  Le N L, Wang Y, Chung T S. Pebax/POSS mixed matrix membranes for ethanol recovery from aqueous solutions via pervaporation[J]. J Membr Sci, 2011, 379(1-2): 174-183.
[29]  孙杰,沈贵.Ag+-13X分子筛吸附汽油中苯并噻吩的性能[J].化工科技,2008,16(5):5-8.
 

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