Xia Yongde, Wang Wenxin, Mokaya Robert
School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, UK.
J Am Chem Soc. 2005 Jan 19;127(2):790-8. doi: 10.1021/ja0453230.
We report the synthesis and characterization of crystal-like structurally well-ordered ethylene-containing hybrid mesoporous organoaluminosilicate materials, which exhibit molecular-level periodicity in the pore walls and enhanced hydrothermal stability. Distilled 1,2-bis(triethoxysilyl)ethylene (BTEE) was used as the organosilica precursor, aluminum isopropoxide as aluminum source, and cetyltrimethylammonium bromide as template. The materials are structurally well-ordered and exhibit high surface area (>1300 m(2)/g) and pore volume (>1.10 cm(3)/g). The presence of molecularly ordered ethylene groups was confirmed by powder X-ray diffraction, (29)Si and (13)C MAS NMR, and Raman spectroscopy. The ethylene groups are thermally stable up to a temperature of 300 degrees C. The presence of ethylene groups enhances the hydrothermal stability in boiling water of both organosilica and organoaluminosilicate materials. The organoaluminosilicate materials possess a bifunctional character arising from the presence of both tetrahedrally coordinated Al and molecularly ordered ethylene groups in their frameworks.
我们报道了晶体状结构有序的含乙烯杂化介孔有机铝硅酸盐材料的合成与表征,这些材料在孔壁中呈现分子水平的周期性,并且具有增强的水热稳定性。蒸馏后的1,2 - 双(三乙氧基硅基)乙烯(BTEE)用作有机硅前驱体,异丙醇铝作为铝源,十六烷基三甲基溴化铵作为模板。这些材料结构有序,具有高比表面积(>1300 m²/g)和孔体积(>1.10 cm³/g)。通过粉末X射线衍射、²⁹Si和¹³C固体核磁共振以及拉曼光谱证实了分子有序乙烯基团的存在。乙烯基团在高达300℃的温度下具有热稳定性。乙烯基团的存在增强了有机硅和有机铝硅酸盐材料在沸水中的水热稳定性。有机铝硅酸盐材料具有双功能特性,这是由于其骨架中同时存在四面体配位的铝和分子有序的乙烯基团。