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- 2015
氧化石墨烯/聚氨酯杂化膜的原位聚合构建及气体渗透性
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Abstract:
采用Hummers法制备了3种不同氧化程度的氧化石墨烯(GO), 通过聚氨酯(PU)单体(4, 4'-二异氰酸苯酯(MDI)和1, 4-丁二醇(BDO))与GO的原位聚合构建了GO/PU杂化膜。利用XRD、Raman、FTIR和TEM等表征了GO的结构; 探讨了GO填充量对GO/PU杂化膜的形貌和CO2、N2渗透性的影响。结果表明:3种不同氧化程度的GO均呈完全剥离状态, 为半透明片状结构; 随着氧化程度的增加, 拉曼D峰与G峰的相对强度比分别为0.947、1.103和1.245; GO的氧化程度对GO在溶剂和杂化膜中的分散性有较大影响, 氧化程度越高, 分散性越好。GO/PU杂化膜的CO2、N2渗透系数及CO2/N2渗透选择因子均随GO填充量的增加先增大后减小; 当中等氧化程度的GO(M-GO)与(MDI+BDO)的质量比为1.0%时, M-GO/PU杂化膜的CO2渗透系数为63.6×10-13 cm3(STP)/(cm·Pa·s), 其中STP表示标准温度及压力, CO2/N2渗透选择因子可达48.5; 填充适量的GO能显著提高GO/PU杂化膜的CO2渗透性及CO2/N2渗透选择性。 Three kinds of graphene oxide (GO) with different oxidation degrees were synthesized by Hummers method. The GO/polyurethane (PU) mixed matrix membranes were fabricated via in-situ polymerization of PU monomers (Methylene Diphenyl 4, 4'-Diisocyanate (MDI) and 1, 4-Butanediol (BDO)) with GO. The structure of GO was characterized by XRD, Raman, FTIR and TEM etc. The effects of GO filling content on the morphology and permeabilities of CO2 and N2 of GO/PU mixed matrix membranes were discussed. The results reveal that the three kinds of GO with different oxidation degrees present a state of complete stripping, and are translucent sheet structure, and with the increasing of oxidation degree, the relative intensities of D peak to G peak in Raman are 0.947, 1.103 and 1.245. The oxidation degree of GO has greater effects on the dispersibility of GO in solution and mixed matrix membrane, when the oxidation degree is higher, the dispersibility is better. The permeability coeffcients of CO2 and N2 and CO2/N2 permeation selectivity factor of GO/PU mixed matrix membrane increase firstly and then decrease with GO filling content increasing. When the mass ratio of middle oxidation degree GO (M-GO) to (MDI+BDO) reaches 1.0%, the CO2 permeability coefficient of M-GO/PU mixed matrix membrane is 63.6×10-13 cm3(STP)/(cm·Pa·s), STP represents for standard temperature and pressure, and the permeation selectivity factor of CO2/N2 reaches 48.5. The filling of appropriate amount of GO could significantly improve the permeability of CO2 and the CO2/N2 permeation selectivity of GO/PU mixed matrix membrane. 国家自然科学基金(21376218,21076190)
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