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从天然高岭土到 Al-MCM-41 介孔材料的物理化学性质研究。

Investigation of the physicochemical aspects from natural kaolin to Al-MCM-41 mesoporous materials.

机构信息

Department of Inorganic Materials, School of Resources Processing and Bioengineering, Central South University, Changsha, China.

出版信息

J Colloid Interface Sci. 2012 Mar 1;369(1):216-22. doi: 10.1016/j.jcis.2011.12.041. Epub 2011 Dec 20.

Abstract

Aluminum-containing hexagonally ordered mesoporous silica Al-MCM-41 was synthesized by hydrothermal treatment of leached products produced by pre-grinding and subsequent acid leaching of natural kaolin, without addition of silica or aluminum regents. The resulting Al-MCM-41 had a high surface area of 1041 m(2)/g, a pore volume of 0.97 mL/g, and an average pore diameter of 3.7 nm with narrow pore size distribution centered at 2.7 nm. During the synthesis process of Al-MCM-41 from natural kaolin, the evolutions of chemical environments for Si and Al atoms should be emphasized. Wide angle X-ray diffraction (WAXRD), high-resolution transmission electron micrographs (HRTEMs), solid-state magic-angle-spinning nuclear magnetic resonance (MAS NMR), Fourier transform infrared spectroscopy (FT-IR) were used to trace the variations of chemical structures. Pretreatment of grinding and subsequent acid leaching acted as an important role in the whole synthesis process. NMR spectroscopy showed that Q(3) structure (Si(SiO)(3)(OH)), condensed Q(4) framework structure (Si(SiO)(4)), also the octahedral and tetrahedral Al existed in the leached sample and Al-MCM-41, with higher chemical contents of Q(4) structure and the octahedral Al in final product Al-MCM-41 than those in the leached sample. A possible mechanism for the formation of Al-MCM-41 from natural kaolin was suggested.

摘要

采用预磨碎和随后酸浸处理天然高岭土得到的浸出产物为原料,在水热条件下合成了不含硅源和铝源的六方有序介孔硅铝分子筛 Al-MCM-41。所得 Al-MCM-41 具有高比表面积(1041 m(2)/g)、大孔容(0.97 mL/g)和窄孔径分布(平均孔径 3.7nm,孔径分布中心 2.7nm)。在以天然高岭土为原料合成 Al-MCM-41 的过程中,应强调硅和铝原子的化学环境演变。利用广角 X 射线衍射(WAXRD)、高分辨率透射电子显微镜(HRTEM)、固态魔角旋转核磁共振(MAS NMR)和傅里叶变换红外光谱(FT-IR)跟踪化学结构的变化。预磨处理和随后的酸浸在整个合成过程中起了重要作用。NMR 谱表明,在浸出样品和 Al-MCM-41 中存在 Q(3)结构(Si(SiO)(3)(OH))、缩合的 Q(4)骨架结构(Si(SiO)(4))和八面体、四面体 Al,最终产物 Al-MCM-41 中的 Q(4)结构和八面体 Al 的化学含量高于浸出样品。提出了一种由天然高岭土制备 Al-MCM-41 的可能机理。

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