Abstract: | 金屬有機骨架材料(Metal-organic frameworks, MOFs)是一種嶄新的材料,由不同的無機金屬或金屬團簇和有機配位體結合而成不同種類之三維多孔配位材料,如HKUST-1 (CuBTC)、MIL、IRMOFs、ZIFs和UiO等,因其優異的物化特性(如體積小、熱穩定性及傳導性良好、可調控性、高比表面積等)使其應用領域廣泛,諸如氣體儲存、吸附、催化及藥物傳遞等方面,為近年來受國際關注的複合性多孔材料,然因MOFs應用於水體之污染物去除時,不易進行固液分離,因此若能賦予磁性則可大大的提升性能與其應用領域。本研究即是利用超順磁性奈米顆粒(SiO2/Fe3O4, SM)當作載體,然後進一步改質,使其帶有氨基(-NH2)和羧基(-COOH),最終透過超音波震盪進行逐層之液相磊晶法(Layer-by-Layer Liquid Phase Epitaxy, LBL LPE)合成出HKUST-1,以獲得磁性MOF-無機基質複合材料,研究HKUST-1生長週期和超音波輔助的參數,以評估最佳合成條件。透過ASAP、TEM、SEM、FTIR、XRD、SQUID和TGA測定所得到的物理化學性質,探討不同層數對表面官能基、晶相結構及比表面積的影響,並初步研究對亞甲基藍(Methylene blue, MB)和Ni(II)的吸附行為,評價材料之吸附性能。本研究得到的結果證明,此製備方法已經成功開發出磁性HKUST-1,且具有從溶液中吸附MB和Ni(II)的能力。 Metal-organic frameworks (MOFs), also called porous coordination polymers (PCPs), are novel porous coordination materials that combined inorganic metals ions or metal clusters with organic linkers to form one-dimensional, two-dimensional, or three-dimensional structures, such as HKUST-1 (CuBTC), MIL, IRMOFs, ZIFs, and UiO, etc. Recently, MOFs have attracted great attention due to their excellent physicochemical properties, like small size, thermal stability, tunable properties, high surface-area; therefore, they are widely used for the gas storage and adsorption, catalysis, drug delivery, and so on. However, when MOFs are applied to the removal of pollutants in solution, it is not easy to separate MOFs from solution. In order to greatly improve their performance and application field, the MOFs grown on the magnetic carrier possess high potential for easy control and specific usage. In this research, superparamagnetic nanoparticles (SiO2/Fe3O4, SM) were used as carriers, then further modified to possess functional groups of amine (-NH2) and carboxylic acid (-COOH), and finally to synthesis HKUST-1 by ultrasound-assisted layer-by layer liquid phase epitaxy (LBL LPE) to obtain magnetic MOF-inorganic materials. The parameters of growth cycles and ultrasound-assisted period were investigated to evaluate the optimal synthetic condition. Physicochemical properties of obtained materials were determined by ASAP, TEM, SEM, FTIR, XRD, SQUID and TGA. The adsorption behavior of methylene blue (MB) and Ni(II) were investigated to evaluate the adsorption performance of the obtained materials. The resulted obtained in this study indicated that the synthetic route developed in this study have successfully developed the magnetic MOF of HKUST-1 and proven to possess adsorption ability to remove MB and Ni(II) from solution. |