改性氧化石墨烯-PEBA混合基质膜对苯酚/水的 渗透汽化分离性能
作者:吴昊 李治康 伍艳辉
单位: 同济大学 化学科学与工程学院,上海市化学品分析、风险评估与控制重点实验室, 上海 200092
关键词: 渗透汽化;苯酚;氧化石墨烯;双酚A;聚醚胺
出版年,卷(期):页码: 2021,41(6):153-161

摘要:
 本研究分别用聚醚胺(PEA)与双酚A(BPA)对氧化石墨烯(GO)进行改性,再与聚醚嵌段共聚酰胺(PEBA)共混制备获得混合基质膜PEA-GO-PEBA与BPA-GO-PEBA,用于水中低浓度苯酚的渗透汽化分离。红外光谱(FT-IR)和X射线光电子能谱(XPS)测试表明PEA与BPA均成功接枝到GO表面,X射线衍射(XRD)测试表明改性后的GO层间距有所增大,其中BPA-GO的层间距增大较为明显,苯酚吸附实验表明改性后的PEA-GO与BPA-GO对苯酚的吸附性能都有提高,其中BPA-GO对苯酚的吸附容量达147.8 mg/g;苯酚/水渗透汽化实验表明在PEBA中引入两种改性GO均能有效提高膜的渗透汽化性能,其中BPA-GO-PEBA混合基质膜的性能更优,55 ℃时通量与分离因子分别达到308 g/(m2·h)和21.1,与未改性的GO-PEBA混合基质膜相比分别提高了50.2%和88.4%,原因在于改性后的BPA- GO对苯酚的亲和性增强且具有更大的层间距。由不同温度下渗透汽化实验数据和Arrhenius方程计算得到BPA-GO-PEBA混合基质膜对苯酚的渗透活化能为81.0 kJ/mol,高于未改性的GO-PEBA混合基质膜和PEBA空白膜,因而温度升高有利于通量和分离因子的同时提高。
 In this study, two different modified graphene oxides were derived, namely polyether amine modified graphene oxide (PEA-GO) and bisphenol A modified graphene oxide (BPA-GO). The modified GO were filled into PEBA to prepare mixed matrix membranes, and their pervaporation performance for phenol/water separation were investigated. IR and XPS characterization proved that the modifications are successful. XRD results indicated that the interlayer spacing of BPA-GO increased significantly. The modified GO showed improved adsorption for phenol. The adsorption capacity of BPA-GO reached 147.8 mg/g. After filling modified GO, the separation factor and permeation flux of the pervaporation membrane have been improved. The mixed matrix membrane BPA-GO-PEBA had the better pervaporation performance than PEA-GO-PEBA membrane. It had the permeation flux of 308 g/(m2·h)and the separation factor of 21.1 at the temperature of 55℃. Due to the fact that BPA-GO had better phenol adsorption property and increased d-spacing, the flux and separation factor of BPA-GO-PEBA membrane increased by 50.2% and 88.4% respectively, compared with the mixed matrix membrane filling unmodified GO. According to the pervaporation experiments data and Arrhenius equation, the activation energy of phenol permeation was 81.0 kJ/mol, which was higher than that of PEBA blank membrane and the mixed matrix membrane with unmodified GO. Therefore, with the temperature increasing, the separation factor and permeation flux of the mixed matrix membrane BPA-GO-PEBA increased markedly.
吴昊(1995-),男,上海人,硕士研究生,研究方向为渗透汽化.

参考文献:
 [1]Busca G, Berardinelli S, Resini C, et al. Technologies for the removal of phenol from fluid streams: A short review of recent developments[J]. J Hazard Mater. 2008, 160(2-3): 265-288.
[2]尚菊红. 废水中苯酚处理方法研究进展[J]. 辽宁化工. 2019, 48(02): 137-139.
[3]Villegas L, Mashhadi N, Chen M, et al. A Short Review of Techniques for Phenol Removal from Wastewater[J]. Curr Pollut Rep. 2016, 2(3): 157-167.
[4]由涛, 陈龙祥, 张庆文, 等. 脱除废水中挥发性有机化合物的渗透汽化复合膜研究进展[J]. 化工进展,2009, 28(9): 1653-1656.
[5]Ye H, Wang Y, Zhang X, et al. Polyurethane membrane with a cyclodextrin-modified carbon nanotube for pervaporation of phenol/water mixture[J]. J Polym Eng. 2017, 37(5): 449-459.
[6]Kujawski W, Warszawski A, Ratajczak W, et al. Application of pervaporation and adsorption to the phenol removal from wastewater[J]. Sep Purif Technol. 2004, 40(2): 123-132.
[7]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.
[8]Vatani M, Raisi A, Pazuki G. Three-component mixed matrix membrane containing [Hmim][PF6] ionic liquid and ZSM-5 nanoparticles based on poly (ether-block-amide) for the pervaporation process[J]. J Mol Liq. 2019, 277: 471-480.
[9]Choudhari S, Cerrone F, Woods T, et al. Pervaporation separation of butyric acid from aqueous and anaerobic digestion (AD) solutions using PEBA based composite membranes[J]. J Ind Eng Chem. 2015, 23: 163-170.
[10]王敏敏,张新儒,李馨然,等. PEBA/MCM-41杂化膜的制备及其对苯酚/水渗透汽化分离性能的研究[J]. 膜科学与技术. 2015, 35(6): 40-47.
[11]张时雨, 邹昀, 韦藤幼, 等. β-环糊精/聚醚共聚乙酰胺填充膜的制备及渗透汽化分离水中微量苯酚[J]. 化工学报, 2016, 67(11): 4662-4670.
[12]Qian Y L, Zhou C, Huang A S. Cross-linking modification with diamine monomers to enhance desalination performance of graphene oxide membranes[J]. Carbon. 2018, 136: 28-37.
[13]Tang W Y, Lou H, Li Y F, et al. Ionic liquid modified graphene oxide-PEBA mixed matrix membrane for pervaporation of butanol aqueous solutions[J]. J Membr Sci. 2019, 581: 93-104.
[14]Zhang W Z, Jia J, Qiu Y Y, et al. Polydopamine-Grafted Graphene Oxide Composite Membranes with Adjustable Nanochannels and Separation Performance[J]. Adv Mater Interfaces. 2018, 5(8): 1701386.
[15]Li W H, Li J, Wang N X, et al. Recovery of bio-butanol from aqueous solution with ZIF-8 modified graphene oxide composite membrane[J]. J Membr Sci. 2020, 598: 117671.
[16]Konkena B, Vasudevan S. Understanding Aqueous Dispersibility of Graphene Oxide and Reduced Graphene Oxide through pK(a) Measurements[J]. J Phys Chem Lett. 2012, 3(7): 867-872. 
[17]Sun H J, Yang Y H, Huang Q. Preparation and Structural Variation of Graphite Oxide and Graphene Oxide[J]. Integr Ferroelectr. 2011, 128: 163-170.
[18]Xiang M, Li CJ, Ye L. Structure and conformation of polyetheramine in confined space of graphene oxide and its enhancement on the electrically conductive properties of monomer casting nylon-6[J]. Composites Part A APPL S. 2017, 95: 1-11.
[19]Wu Y H, Tian G Q, Tan H F, et al. Pervaporation of phenol wastewater with PVDF-PU blend membrane[J]. Desalin Water Treat. 2013, 53: 5311-5318.
[20]Bakhshi A, Mohammadi T, Aroujalian A. Pervaporation separation of binary and ternary mixtures with polydimethylsiloxane membranes. J Appl Polym Sci 2008, 107 (3): 1777-1782
[21]Wu Y H, Fu X T , Tian G Q, et al. Pervaporation of phenol wastewater with PEBA-PU blend membrane[J]. Desalin Water Treat. 2018, 102: 101-109.
[22]Ye H, Yan X, Zhang X, et al. Pervaporation properties of oleyl alcohol-filled polydimethylsiloxane membranes for the recovery of phenol from wastewater[J]. Iran Polym J. 2017, 26(8): 639-649.
[23]Li D, Yao J, Sun H, et al. Preparation and characterization of SiO2/PDMS/PVDF composite membrane for phenols recovery from coal gasification wastewater in pervaporation[J]. Chem Eng Res Des. 2018, 132: 424-435.
[24]Feng X S, Huang RYM. Estimation of activation energy for permeation in pervaporation processes[J]. J Membr Sci. 1996, 118(1): 127-131.

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