化工学报 ›› 2017, Vol. 68 ›› Issue (5): 2177-2185.DOI: 10.11949/j.issn.0438-1157.20161673

• 材料化学工程与纳米技术 • 上一篇    下一篇

氧化石墨烯-陶瓷复合纳滤膜的层层自组装制备及其性能

高克1, 许中煌1, 洪昱斌3, 丁马太1, 何旭敏2, 蓝伟光1,3   

  1. 1 厦门大学材料学院, 福建 厦门 361005;
    2 厦门大学化学化工学院, 福建 厦门 361005;
    3 三达膜科技(厦门)有限公司, 福建 厦门 361022
  • 收稿日期:2016-11-28 修回日期:2017-01-16 出版日期:2017-05-05 发布日期:2017-05-05
  • 通讯作者: 何旭敏,蓝伟光

Layer-by-layer self-assembly preparation and performance of GO-ceramics composite nanofiltration membrane

GAO Ke1, XU Zhonghuang1, HONG Yubin3, DING Matai1, HE Xumin2, LAN Weiguang1,3   

  1. 1 College of Materials, Xiamen University, Xiamen 361005, Fujian, China;
    2 College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China;
    3 Suntar Membrane Technology (Xiamen) Co., Ltd., Xiamen 361022, Fujian, China
  • Received:2016-11-28 Revised:2017-01-16 Online:2017-05-05 Published:2017-05-05

摘要:

氧化石墨烯(GO)的片层边缘含有 COOH等含氧官能团,因而带负电荷,可以在带正电荷多孔基体上通过层层自组装实现快速沉积。以由3-氨丙基三乙氧基硅烷(APTES)修饰的多孔氧化铝管式陶瓷膜为基膜,令GO和聚乙烯亚胺(PEI)以溶液形态在其表面交替沉积实现自组装,继以环氧氯丙烷(ECH)交联之,制备新型氧化石墨烯-陶瓷复合纳滤膜。最佳制备工艺是,PEI浓度5 g·L-1、pH=9,NaCl浓度0.3 mol·L-1,GO浓度0.6 mg·ml-1、pH 4.5,层数2层,ECH用量6.25 ml·L-1,50℃条件下处理70 min。层数为1~4层的自组装膜在0.6 MPa操作压力下对2 g·L-1的MgCl2的截留率分别为90.16%、93.71%、97.54%、92.93%,其中1层自组装膜的渗透通量为21.92 L·m-2·h-1。氧化石墨烯-陶瓷复合纳滤膜对4种无机盐的截留率大小为MgCl2 >MgSO4 > NaCl >Na2SO4,符合典型正电荷纳滤膜的特征。

关键词: 氧化石墨烯, 层层自组装, 纳滤, 荷正电, 膜, 过滤

Abstract:

Graphene oxide (GO) can be quickly deposited on a positively charged porous matrix via a layer-by-layer self-assembly strategy because GO nanosheets contain rich negatively charged, oxygen-containing function groups, such as COOH. In this paper, the GO-ceramics composite nanofiltration membrane was prepared via layer-by-layer deposition of GO solution and eolyethyleneimine (PEI) solution alternately, and then cross-linked by epoxy chloropropane (ECH) on 3-aminopropyltriethoxysilane-modified porous Al2O3 supports. The optimum preparation conditions were: PEI 5g·L-1, pH=9; NaCl 0.3 mol·L-1; GO 0.6 mg·L-1, pH 4.5; ECH 6.25 ml·L-1 and heat treatment 50℃/70 min. Under the conditions of 0.6 MPa, when the self-assembly layer number increased from 1 to 4, the rejection to 2 g·L-1 MgCl2 were 90.16%, 93.71%, 97.54%, and 92.93% respectively,and the flux of self-assembled monolayer membrane was 21.92 L·m-2·h-1. The rejection orders of inorganic salts of GO-ceramics composite nanofiltration membrane were as follows: MgCl2 >MgSO4 >NaCl >Na2SO4, therefore they showed the typical positively charged nanofiltration membrane characteristics.

Key words: graphene oxide, layer-by-layer self-assembly, nanofiltration, positively charged, membrane, filtration

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