Enhanced butanol selectivity of pervaporation membrane with fluorinated monolayer on polydimethylsiloxane surface
Enhanced butanol selectivity of pervaporation membrane with fluorinated monolayer on polydimethylsiloxane surface
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聚二甲基硅氧烷表面氟化单层渗透汽化膜增强丁醇选择性
DOI：
10.1016/j.memsci.2017.11.015
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发表时间：
2018-02
影响因子：
9.5
通讯作者：
An Quan-Fu
中科院分区：
文献类型：
--
作者：
Zheng Pei-Yao;Li Xiao-Qing;Wu Jia-Kai;Wang Nai-Xin;Li Jie;An Quan-Fu
以氟烷基硅烷(FAS)为交联剂，在聚二甲基硅氧烷(PDMS)膜表面制备了氟化分子单分子膜。具体而言，将端羟基PDMS与1H，1H，2H，2H-全氟十二烷基三乙氧基硅烷进行交联，然后浇铸在多孔聚砜载体上，制得PDMS膜。X-射线光电子能谱分析表明，氟化烷基链在膜的表面有丰富的分布。此外，随着Fas含量的增加，薄膜表面的氟含量也随之增加，当表面被氟化单分子膜完全覆盖时，氟含量稳定在55at%左右(接近Fas分子的含量)。水接触角测量表明，表面疏水性与表面氟含量成正比。在60℃下对1wt%正丁醇/水混合物进行渗透汽化分离时，乙氧基与羟基当量比为35(PdMS-Fas-35)的膜的渗透通量为843g−2 h−1，与传统正硅酸乙酯(1 375g−2 h−1，24.4wt%)相比，渗透丁醇浓度提高了34.3wt%。渗透通量的降低是由于水膜部分通量的减小，而不牺牲正丁醇的部分通量，从而导致了Fas单层的拒水性能。结果表明，Fas交联型PDMS可以提高膜的分离效率，从而降低渗透汽化过程的成本和能耗。
A facile approach to fabricate fluorinated molecular monolayer on the surface of polydimethylsiloxane (PDMS) membrane was conducted using fluoroalkylsilane (FAS) as cross-linking agent. In detail, hydroxyl terminated PDMS were cross-linked with 1H,1H,2H,2H-Perfluorodecyltriethoxysilane and cast on porous polysulfone support to prepare PDMS membranes. X-ray photoelectron spectroscopy showed that fluorinated alkyl chains were enriched at the surface of the membranes. Moreover, the surface fluorine concentration increased with the increasing of FAS and plateaued at around 55 at% (close to that of FAS molecules) when the surface was fully covered by fluorinated monolayers. The surface hydrophobicity was proportional to the surface fluorine content as revealed by water contact angle measurement. When applied in pervaporation separation of 1 wt%n-butanol/water mixture at 60 °C, the membrane prepared with a FAS ethoxy to PDMS hydroxyl equivalents ratio of 35 (PDMS-FAS-35) exhibited a flux of 843 g−2h−1and an enhanced permeaten-butanol concentration of 34.3 wt% compared with PDMS cross-linked with traditional TEOS (1375 g−2h−1, 24.4 wt%). The decrease of permeate flux was because of the reduced water partial flux without sacrificing the butanol partial flux on the consequence of water repellency of FAS monolayer. The results indicated that the FAS cross-linked PDMS could increase the separation efficiency of the membrane, thereby reducing the cost and energy consumption of the pervaporation process.
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