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Immobilized Manganese-porphyrin and Molybdenum-Schiff Base Complexes on Functionalized Magnetic Nanoparticles as Efficient Recyclable Nanocatalysts in Hydrocarbon and Sulfide Oxidation Reactions

Mortazavi Manesh, Anahita | 2017

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  1. Type of Document: Ph.D. Dissertation
  2. Language: Farsi
  3. Document No: 49827 (03)
  4. University: Sharif University of Technology
  5. Department: Chemistry
  6. Advisor(s): Bagherzadeh, Mojtaba
  7. Abstract:
  8. In this thesis, functionalized Fe3O4 nanoparticles have been utilized as a support for immobilization of homogeneous catalysts. The catalytic activity of the supported heterogeneous nanocatalysts was investigated in hydrocarbon and sulfide oxidation reactions. In the first part of this research, imidazole functionalized Fe3O4 nanoparticles (Fe3O4@SiO2-Im) were used as a support to anchor manganese porphyrin complex, [MnT(4-OMeP)P]OAc; via axial ligation. Catalytic application of the immobilized manganese porphyrin was studied in oxidation of alkenes and sulfides. To find suitable reaction conditions, the effect of different parameters such as solvent and temperature on immobilization process and also various reaction parameters (oxidant, solvent, and time) on oxidation reactions has been investigated. The synthesized nanocatalyst could be magnetically separated and reused multiple times without significant loss of catalytic activity. In the second part, covalent immobilization of manganese porphyrin, [Mn(TPFPP)OAc]; on silica-coated magnetic nanoparticles functionalized with 3-aminopropyltriethoxysilane (APTS) was carried out through the amino propyl linkage. The immobilized manganese porphyrin was applied as an efficient and retrievable nanocatalyst in alkane oxidation and alkene epoxidation. Stability and recycling experiments revealed that the synthesized nanoparticles could be reused several times without loss of catalytic activity and magnetic properties. In the next part of this study, functionalized MNP@PMA nanoparticles containing a molybdenum Schiff base complex were prepared using a few consecutive steps. Application of the heterogenized nanocatalyst was studied in epoxidation of olefins. To find suitable reaction conditions, the effect of parameters such as solvent and catalyst amount has been investigated in oxidation reactions. It should be mentioned that high surface area of these nanoparticles could obtain high loadings of catalytically active sites. The MNP@PMA-SB-Mo nanocatalyst could be magnetically separated and reused multiple times without significant loss of catalytic activity. In the fourth part, manganese porphyrin complex immobilized on magnetic nanoparticles coated imidazole base type polymer (MNP@GMA-Im) via axial ligation. Application of the immobilized manganese porphyrin on the functionalized magnetic nanoparticles as a heterogenized nanocatalyst in oxidation of alkenes was studied. Recycling experiment revealed that the synthesized nanoparticles could be reused several times without loss of catalytic activity and magnetic properties. Thus, the nanocatalysts with high catalytic activity (in term of TON), high stability and easy recyclability were prepared in this thesis. In other words, these heterogenized catalytic systems could join the catalytic properties of the homogeneous catalysts with the magnetic properties of Fe3O4 nanoparticles
  9. Keywords:
  10. Nano Catalyst ; Magnetic Nanodot ; Manganese-Porphyrin Complexes ; Oxidation ; Molybdenum Schiffbase Complex ; Sulfide Oxidation

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