Chuiko Institute of Surface Chemistry of NAS of Ukraine, 17 General Naumov Str., Kyiv 03164, Ukraine.
Chuiko Institute of Surface Chemistry of NAS of Ukraine, 17 General Naumov Str., Kyiv 03164, Ukraine.
J Environ Sci (China). 2021 Jan;99:59-71. doi: 10.1016/j.jes.2020.04.027. Epub 2020 Jun 27.
Organosilicas with chemically immobilized 3-aminopropyl and Methyl Red-containing surface groups were prepared by sol-gel condensation of tetraethyl orthosilicate and (3-aminopropyl)triethoxysilane in the presence of dye as part of the mixed micelles or dye-containing silane as silica source. The hexagonally arranged mesoporous structure of synthesized materials was confirmed by low-temperature nitrogen adsorption-desorption, x-ray diffraction, and TEM studies. Chemical composition of MCM-41-type organosilicas was established by FT-IR spectroscopy and chemical analysis of surface layer. Sorption of Methyl Red by organosilicas was studied from diluted phosphate buffer solutions in dependence of medium pH, duration of contact, and equilibrium concentration of dye. It was found that effective removal of Methyl Red takes place at pH values within a range of 2.5-5. Kinetic curves of Methyl Red sorption on organosilicas were analyzed by the Lagergren, Ho-McKey, and Weber-Morris kinetic models. It was found that the pseudo-second-order model fits the kinetics of Methyl Red sorption on all synthesized materials and the intraparticle diffusion is not the only one mechanism controlling the rate of Methyl Red sorptive removal. The parameters of equilibrium sorption of Methyl Red on organosilicas of MCM-41 type were calculated using Langmuir, Freundlich, Redlich-Peterson, and Brunauer-Emmett-Teller models. Sorption of acid dyes with geometry similar or substantially different from Methyl Red on mesoporous silicas was studied from single and binary component mixtures in aqueous solutions with pH 4.8 and 5.5. It was found that selective sorption process is highly dependent on the structural characteristics and protolytic state of silica surface as well as acid dye.
采用正硅酸乙酯和(3-氨丙基)三乙氧基硅烷在染料存在下作为混合胶束的一部分或作为硅源的含染料硅烷进行溶胶-凝胶缩合,制备了化学固定化 3-氨丙基和甲基红表面基团的有机硅。通过低温氮吸附-解吸、X 射线衍射和 TEM 研究证实了合成材料具有六方排列的介孔结构。通过 FT-IR 光谱和表面层的化学分析确定了 MCM-41 型有机硅的化学组成。研究了在不同的介质 pH 值、接触时间和染料平衡浓度的条件下,从稀释的磷酸盐缓冲溶液中吸附甲基红。结果表明,在 pH 值为 2.5-5 的范围内,有效去除了甲基红。通过 Lagergren、Ho-McKey 和 Weber-Morris 动力学模型分析了甲基红在有机硅上的吸附动力学曲线。结果表明,准二级模型拟合了所有合成材料上甲基红吸附的动力学,内扩散不是控制甲基红吸附去除速率的唯一机制。采用 Langmuir、Freundlich、Redlich-Peterson 和 Brunauer-Emmett-Teller 模型计算了 MCM-41 型有机硅对甲基红的平衡吸附参数。在 pH 值为 4.8 和 5.5 的水溶液中,研究了与甲基红几何形状相似或差异较大的酸性染料在介孔硅上的单组分和双组分混合物中的吸附。结果表明,选择性吸附过程高度依赖于二氧化硅表面的结构特征和质子化状态以及酸性染料。