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Synthesis, Functionalization And Encapsulation Of Mesoporous Materials

Posted on:2007-09-16Degree:MasterType:Thesis
Country:ChinaCandidate:J LiFull Text:PDF
GTID:2121360185454625Subject:Inorganic Chemistry
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As a new kind of host-guest materials, mesoporous materials received much attention. With ordered nano-scope pores and easily adorned inner surface, mesoporous materials can be further processed. Adorned by physical and chemical method, the chemistry environments of their inner surface can be adjusted, becoming a better host-material for assembling other functional materials. After adorned, the property of mesoporous materials and guest-materials can become uniform, so the guest materials can be assembled in the inner surface. The host-guest complex materials obtained by this method have both the property of mesoporous materials and that of guest materials, which includes both their own property and the properties occurred under the quantum scale effect, so they are a kind of functionalized mesoporous materials with excellent performance, offering a broad research field for adjusting their properties in molecule or nanometer scope. Meanwhile, the research for the structures of different surfactants and the relationship between their structure directing effects and the structure of mesopours materials can lead occurrence of both novel structure directing agents and novel mesoporous materials, and this process can broad the application of mesoporous materials too. After usage of anionic surfactant, the synthesis of mesoporous materials by using it became a new hotspot, meanwhile the occurrence of helical structure mesoporous materials made it a new hotspot too.Aiming at the problems existed in the research of mesoporous materials, in this dissertation, we studied some aspects below. Studied both the synthesis of mesoporous materials by anion surfactant and that with helical structureporous. Adorned the inner tunnels of mesoporous material SB A-15 by PAMAM;studied the property of adorned SBA-15.In the first part, we used anionic surfactant sodium laruoyl glutamate as structure directing agent, studied the different structures obtained by 3-aminopropyl-trimethoxysilane and N-aminoethane-3-aminopropyl-trimethoxysilane as co-structure-directing agent (CSDA) respectively. The usage of CSDA 3-amino-propyltrimethoxysilane can cause a Pm3n structure, but due to a larger effective area of the CSDA N-aminoethane-3-aminopropyl-trimethoxysilane can make the Pm3n structure disappear and cause the total structure disordered. This was characterized by the X-ray diffraction (XRD), the nitrogen adsorption/desorption and the TEM. In the same part, we designed a cationic surfactant with a chiral hydrophilic group, synthesized it in a four-step reaction and monitored the purity and yield by HPLC-MS except the last quaternizing step. The XRD pattern of the sample synthesized by this surfactant proved it a 2D hexagonal P6mm structure. The images of SEM proved that the sample has a helical morphology, but without the proof of the TEM images. Then we tried to explain the formation mechanism of helical structure mesoporous materials. While using the AAO as template for the synthesis of helical mesoporous materials, we prepared nano-scope zeolite MFI without the template molecule TPAOH and the process of hydrothermal. The scope of MFI was about 200nm, nearly the same as the diameter of AAO pores, so the scope can be controlled by the AAO with different pore diameter.In the last part, we adorned the porous wall of mesoporous material SBA-15 with amine group, made it full of amine center, then using the method reported in reference, through repeated Michael addition with methyl acrylate and amidationwith ethylenediamine, the dendrimer poly-amino-amine (PAMAM) was grafted on the surface of SB A-15 tunnels. We characterized the adorned degree of the sample by nitrogen adsorption/desorption, infra-red and TGA. The adorning made SBA-15 tunnels more amine groups and nano-scope matrix with higher coordinative ability. Then we used the adorned SBA-15 as host. Due to full of amine in the surface of PAMAM, we encapsulated the Coumarin 4 in the tunnels of adorned SBA-15, and studied the fluorescence property of the samples with different Coumarin 4 concentration. Through the ion exchange, coordination and reduction method, we obtained a kind of composite with nickel-nanoparticles in the tunnels of PAMAM adorned SBA-15. Due to coordinative ability between nickel ion and PAMAM, and the confinement of PAMAM nano-matrix and SB A-15 mesopores, we encapsulated nickel-nanoparticles in the pores. The characterization of UV-Visable and nitrogen adsorption/desorption helped prove the existence of nickel-particles in the pores with nano-scope.
Keywords/Search Tags:Functionalization
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