硅钨基多金属氧酸盐催化剂的合成、表征及催化应用-化学 物理化学专业论文.docxVIP

AbstractPolyoxometalates Abstract Polyoxometalates are a虹nd of inorganic compounds which are well known by people．The compounds have been received more and more attention in the area of catalysis in recent years，because they are economical and environmentally friendly catalysts with high catalytic performance and selectivity．Their acidic and redox properties Call be controlled at atomic or molecular levels．Therefore， polyoxometalates are capable of catalyzing oxidation reaction．The main progress and research results in the paper have been obtained as follows： 1．Peroxotungstate【DDA]3[(OH)Si03{WO(02)2}3】as catalyst for epoxidation of alkenes This paper reported a new peroxotungstate【DDA]3[(OH)Si03{WO(02)2}3】(I)， which Was synthesized and used as reaction·-controlled phase--transfer catalyst for epoxidation of alkenes with H202 as the oxidant and ethyl acetate as the solvent epoxidation systems．This system can be used for catalytic epoxidation of olefins and exhibits high converSion and selectivity．In an H20／ethyl acetate biphasic system， catalyst I itself was not soluble in the ethyl acetate phase，but it dissolved slowly with the increase of reaction temperature and action of hydrogen peroxide and olefin， which subsequently led to homogeneous catalytic epoxidation of olefins．When the reaction stopped，the structure of catalysts had changed with the transfer of active oxygen of catalyst and consumption of hydrogen peroxide．Wim temperature dropping， catalyst I precipitated gradually．This new system not only catalyzed homogeneous epoxidation of alkenes with unique reaction·-controlled phase·-transfer catalyst character,but also avoided the using of toxic solvents．The catalyst could be easily recovered and reused after reaction，and the epoxidation of cyclohexene Was recycled twenty times without activity loss．The fresh catalyst，used one were characterized by ICP,IR,UV-vis，1 83W NMR and 29Si MAS NMR．· 2．Substituted Keggin—polyoxometalate complexes as catalyst for the select