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Development of mesoporous structure of metals and organometallic catalyst and its catalytic properties of organic reaction in aqueous medium

Author: YinJieZuo
Tutor: LiHeXing
School: Shanghai Normal University
Course: Industrial Catalysis
Keywords: Sonogashira reaction Ullmann reaction Aqueous media Green Chemistry The mesoporous metal and the organometallic catalyst Surface functionalization
CLC: O643.32
Type: Master's thesis
Year: 2009
Downloads: 82
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Abstract


Increasingly serious global environmental pollution problems caused by the concept of \At the same time, the authority chemical research institutions and chemists began to realize that the chemistry and the chemical industry of the serious pollution of the environment, green chemistry came into being. At its heart is the \In 1992, Mobil was first reported ordered mesoporous silicalite, ordered mesoporous materials become the research hotspot. Its large surface area, ordered mesopores and rich surface chemical properties important for the design of efficient heterogeneous catalyst carrier. Around the purpose of green chemistry, through the development of new and efficient heterogeneous catalyst, carried out in an aqueous medium clean organic synthesis, to achieve repeated use of the catalyst on the one hand, to reduce the cost, on the other hand, the reduction of heavy metal ions and organic solvents on the environment pollution. The research is the synthesis of a series of organic functional groups modified ordered mesoporous silica materials with different pore morphology, then metal nanoparticles or organic metal compounds immobilized in the pore, prepared a new mesoporous structure of metals and organic metal catalyst, and investigated the catalytic performance of different types of organic reactions in aqueous media, combined with characterization and kinetic determination of the catalytic reaction mechanism and catalyst structure-activity relationships. By the copolymerization step self-assembly synthesis phenyl, amino common modified SBA-15, as the carrier prepared mesoporous structure supported Pd catalyst Pd / NH 2 Ph- SBA-15 and applied iodine the benzene synthesis of biphenyl in aqueous medium Ullmann-type carbon-carbon coupling reactions. Studies have shown that, the carrier still maintain phenyl, amino-functionalized mesoporous structure and catalytic performance is significantly better than Pd / SiO 2 Pd/SBA-15, Pd/Ph-SBA-15 and Pd / NH 2 -SBA-15, due to the highly dispersed distribution of enhanced surface hydrophobicity and Pd particles on the carrier. Methylene bridged the organosilane synthetic PMO type Ordered mesoporous materials, the introduction of the silane containing the Si-H bond to the grafting method, the Si-H in the active H situ reduction of Pd / H-PMO (Ph. ) catalyst. Methylene bridged silane assembled into the mesoporous carrier phenyl group (s) uniformly embedded in the hole wall so that the entire material having a great deal of the hydrophobic properties, while avoiding the introduction of a phenyl group in the inorganic carrier to a certain extent destroy tacticity bore structure. Situ reduction of Pd ions to be able to obtain a more uniform distribution of Pd nanoparticles, display high activity and selectivity, as well as good service life in the Synthesis of iodobenzene biphenyl Ullmann-type carbon-carbon coupling reaction in an aqueous medium. 3 under acidic conditions in the use of non-ionic surface active agent of P123, use of the organic silane and TEOS with diphenylphosphine, ethyl bridged or Methylene bridged silane copolycondensate, synthetic diphenylphosphine ( PPh 2 -) modified ordered mesoporous materials, and then a covalent bond anchoring organometallic catalyst Ni (PPh 3 ) 2 Cl 2 immobilized in the pore. Iodobenzene and phenylacetylene of the catalyst prepared in an aqueous medium Sonogashira carbon-carbon coupling reactions show good activity and selectivity, and can be used repeatedly. The new method developed in this paper can be extended to the preparation of the of mesoporous metal and organometallic catalyst, also making multifunctional catalyst, help to promote the application and popularization of clean design and industrialization of organic synthesis reaction in aqueous medium.

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CLC: > Mathematical sciences and chemical > Chemistry > Physical Chemistry ( theoretical chemistry ),chemical physics > Chemical kinetics,catalysis > Catalytic > Catalytic reaction
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