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The Applications Of Ordered Mesoporous Materials In The Adsorption Of Organic Pollutants And Catalysis

Posted on:2014-01-05Degree:MasterType:Thesis
Country:ChinaCandidate:B LiFull Text:PDF
GTID:2231330395991099Subject:Organic Chemistry
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In20th Century90s, Kresge and Beck of American Mobil Oil Company developed a kind of novel porous material during the work of investigating catalyst for oil refining. This kind of materials was named M41S mesoporous materials. According the regulation of IUPAC, mesoporous materials have a pore size distribution between2and50nm. Mesoporous materials have the properties like tunable pore size, abundant silanol group, high surface area and volume and controllable morphology (ball, rod, film, sheet.etc), which makes them have a great potential application in catalysis, biology, water treatment, energy and optics. Water pollution caused by chemical industrial production and daily life has become a significant enviromental issue. And the research for resolving pollution caused by chemical industrial production and daily life will be a focus.In chapter1, there is a comprehensive description of mesoporous materials, including the mechanism of formation, categories and applications. Meanwhile, we have a discussion about the application of mesoporous materials in practical production.In chapter2, mesoporous micelle@silica hybrid materials with2D hexagonal mesostructures were synthesized as reusable sorbents for hydrophobic organic compounds (HOCs) removal by a facile one-step aqueous solution synthesis using3-(trimethoxysily)propyl-octadecyldimethyl-ammonium chloride (TPODAC) as a structure directing agent. The mesopores were generated by adding micelle swelling agent,1,3,5-trimethylbenzene, during the synthesis and removing it afterward, which was demonstrated to greatly increase the HOC removal efficiency. In this material, TPODAC surfactant is directly anchored on the pore surface of mesoporous silica via-Si-O-Si-covalent bond after the synthesis due to its reactive-Si-(OCH3)3head group, and thus makes the synthesized materials can be easily regenerated for reuse. The obtained materials show great potential in water treatment as pollutants sorbents.In chapter3, supported metal oxides were synthesized. Supported metal oxides has the advantages of ease handling and high catalytic efficiency of active center. We reported a general strategy for the preparation of well dispersed CuFe2O4supported on mesoporous silica. A pre-drying step was used before calcination to avoid phase separation and aggregation and to control the dispersion of metal oxides nanoparticles. This facile step can also be extended to NiFe2O4, CuCr2O4, CoFe2O4and all materials obtained are well-dispersed. Supported CuFe2O4was used to the catalytic reaction of asymmetric hydrosilylation of aryl ketone. The yield and ee value can reach93%and93%, respectively. The catalytic performance is better than homogeneous Cu(OAc)2·H2O catalyst and can be recycled by external magnetic field.In chapter4, mesoporous Co3O4was synthesized via nanocasting method. Different pore size mesoporous silica was synthesized and they will act as mother template. Iron nitrate was added to the precursor during the preparation of Co3O4to make a kind of material with superparamagnetic property. Then the synthesized material was used to catalyze the reaction of4-nitroacetophenone. The conversion and ee value are99.5%and88.9%, respectively. In comparison with homogeneous catalyst Co(OAc)2-4H2O, the catalytic performance of heterogeneous catalyst is approximately the same as homogeneous. Above all, the heterogeneous catalyst can be recycled by external magnetic field and reused without losing catalytic property. This magnetic property can avoid the pollution caused by leaching of metal ion.
Keywords/Search Tags:mesoporous materials, impregnation method, nanocasting, water treatment, asymmetric catalysis
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