Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology , Beijing 100029, China.
ACS Appl Mater Interfaces. 2017 Jan 18;9(2):1710-1718. doi: 10.1021/acsami.6b14371. Epub 2017 Jan 5.
Graphene oxide (GO) membranes assembled by single-atom thick GO nanosheets have displayed huge potential application both in gas and liquid separation processes due to its facile and large-scale preparation resulting from various functional groups, such as hydroxyl, carboxyl, and epoxide groups. Taking advantage of these characters, GO membranes intercalated by superhydrophilic metal-organic frameworks (MOFs) as strengthening separation fillers were prepared on modified polyacrylonitrile (PAN) support by a novel pressure-assisted self-assembly (PASA) filtration technique instead of traditional vacuum filtration method for the first time. The synthesized MOF@GO membranes were characterized with several spectroscopic techniques including X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), as well as scanning electron microscopy (SEM). Compared with GO membrane, these MOF@GO membranes combine the unique properties of MOF and GO and thus have significant enhancements of pervaporation (PV) permeation flux and separation factor simultaneously for ethyl acetate/water mixtures (98/2, w/w) through the PV process, which are also superior to the reported other kinds of membranes. Especially, for MOF@GO-0.3 membrane (corresponding MOF loading: 23.08 wt %), the increments are 159% and 244%, respectively, at 303 K, and the permeate water content can reach as high as 99.5 wt % (corresponding separation factor, 9751) with a high permeation flux of 2423 g m h. Moreover, the procedures of both the synthesis of MOF and membranes preparation are environmentally friendly that only water was used as solvent. Such a nanosized MOF-intercalating approach may be also extended to other laminated membranes, providing valuable insights in designing and developing of advanced membranes for effective separation of aqueous organic solution through nanostructure manipulation of the nanomaterials.
氧化石墨烯(GO)膜由单层 GO 纳米片组装而成,由于其具有各种官能团,如羟基、羧基和环氧基,易于大规模制备,因此在气体和液体分离过程中显示出巨大的潜在应用。利用这些特性,通过一种新颖的压力辅助自组装(PASA)过滤技术,在改性聚丙烯腈(PAN)支撑体上制备了由超亲水金属-有机骨架(MOF)作为增强分离填料插层的 GO 膜,而不是传统的真空过滤方法。采用 X 射线衍射(XRD)、傅里叶变换红外光谱(FTIR)、X 射线光电子能谱(XPS)和扫描电子显微镜(SEM)等多种光谱技术对合成的 MOF@GO 膜进行了表征。与 GO 膜相比,这些 MOF@GO 膜结合了 MOF 和 GO 的独特性质,因此在乙基乙酸酯/水混合物(98/2,w/w)的渗透蒸发(PV)过程中同时显著提高了渗透通量和分离因子,优于已报道的其他类型的膜。特别是对于 MOF@GO-0.3 膜(相应的 MOF 负载量:23.08wt%),在 303K 时,分别增加了 159%和 244%,渗透水含量高达 99.5wt%(相应的分离因子为 9751),渗透通量为 2423gmh。此外,MOF 合成和膜制备过程都很环保,只用水作为溶剂。这种纳米级 MOF 插层方法也可以扩展到其他层状膜,为通过纳米材料的结构调控有效分离水相有机溶液的先进膜的设计和开发提供了有价值的见解。