Synthesis and Characterization of Periodic Mesoporous Organosilica Materials

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dc.contributor.author Tshavhungwe, Alufelwi Maxwell
dc.date.accessioned 2006-11-15T07:32:33Z
dc.date.available 2006-11-15T07:32:33Z
dc.date.issued 2006-11-15T07:32:33Z
dc.identifier.uri http://hdl.handle.net/10539/1722
dc.description Student Number : 0107507J - PhD thesis - School of Chemistry - Faculty of Science en
dc.description.abstract Periodic mesoporous organosilica (PMO) materials (consisting of ethane groups in the framework) and bifunctional periodic mesoporous organosilica materials (consisting of ethane groups in the framework and either glycidoxypropyl groups or aminopropyl groups in the channels) were synthesized by the sol-gel method under basic conditions. Ethanesilica materials were synthesized by condensation of 1,2-bistrimethoxysilylethane (BTME) and by co-condensation of BTME with tetraethylorthosilicate (TEOS). Bifunctional periodic mesoporous organosilica materials were synthesized by the co-condensation of BTME with either 3- glycidoxypropyltriethoxysilane (GPTS) or 3-aminopropyltriethoxysilane (APTS). Cetyltrimethylammonium bromide was used as the structure-directing template. Cobalt ion incorporated ethanesilica and modified ethanesilica materials were synthesized in situ by adding cobalt nitrate to the reaction mixture. Cobalt was also supported on ethanesilica materials and APTS-modified materials by using the incipient wetness impregnation method. Raman spectroscopy and diffuse reflectance infrared spectroscopy (DRIFTS) results confirmed the formation of organosilica materials and showed that the surfactant was removed by solvent extraction. Thermogravimetric analysis (TGA) and differential thermal analysis (DTA) showed that the ethane portion of the materials (originating from the bridging ethane group in BTME) only decomposed at temperatures > 400 oC. These techniques also showed that the surfactant is removed by solvent extraction. Cobalt ion incorporation was confirmed by Raman spectroscopy and UV-vis diffuse reflectance spectroscopy. Powder powder X-ray diffraction (XRD) and nitrogen adsorption data indicated that the mesophase and textural properties of the materials are dependent on the reaction conditions (i.e. ageing duration, ageing temperature, amount of silica precursor(s), amount of water and amount of base (NH4OH)). The periodicity of the materials was indicated by the presence of low angle diffraction peaks in powder X-ray diffraction patterns. Cubic and hexagonal mesophases were identified using powder X-ray diffraction. When solvent extraction is prolonged, the BET surface area and the pore volume increase, while the average pore diameter decreases. Materials with more dominant XRD structural features and larger d values, higher surface areas, lower pore volumes and average pore diameters are obtained when low ageing temperatures are used. For samples prepared from a mixture of BTME and TEOS at a given temperature, the surface area was found to increase with increasing amount of TEOS added. This trend was observed for materials with and without cobalt. Type IV isotherms, typical of mesoporous materials, were obtained for ethanesilica and modified ethanesilica materials prepared without cobalt. For cobalt incorporated periodic mesoporous ethanesilica materials, the XRD lattice parameter (d100) increased whereas surface area and pore volume decreased with increasing cobalt loading. Nitrogen gas adsorption on samples with varying ratios of BTME:GPTS or BTME:APTS revealed that increasing the amount of GPTS or APTS affects pore size, surface area and pore volume as well as shapes of the isotherms and hysteresis loops. The hysteresis loops of the Type IV isotherms obtained for GPTS-modified ethane silica materials (without cobalt) change from Type H3 to Type H4. There is a tendency for pore sizes to change from mesopore to micropore when the amount of GPTS is increased. Isotherms of cobalt incorporated GPTS-modified ethane silica materials changed from Type IV to Type I. The surface area, pore volume and pore diameter decreased with increasing loading of GPTS or APTS as well as after cobalt incorporation. en
dc.format.extent 4721910 bytes
dc.format.mimetype application/pdf
dc.language.iso en en
dc.subject periodic mesoporous organosilica en
dc.subject ethanesilica en
dc.subject cobalt incorporation en
dc.title Synthesis and Characterization of Periodic Mesoporous Organosilica Materials en
dc.type Thesis en


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