Hybrid polyoxotungstate/MIL-101 materials: synthesis, characterization, and catalysis of H2O2-based alkene epoxidation.

作者: Nataliya V. Maksimchuk , Konstantin A. Kovalenko , Sergey S. Arzumanov , Yurii A. Chesalov , Maxim S. Melgunov

DOI: 10.1021/IC902459F

关键词:

摘要: Polyoxotungstates [PW4O24]3− (PW4) and [PW12O40]3− (PW12) have been inserted into nanocages of the metal organic framework MIL-101. The hybrid materials PWx/MIL-101 (x = 4 or 12) containing 5−14 wt % polyoxotungstate obtained characterized by elemental analysis, N2 adsorption, FT-IR, Raman, 31P NMR MAS spectroscopic techniques. Their catalytic performance was assessed in selective oxidation alkenes with aqueous hydrogen peroxide under mild reaction conditions ([H2O2] 0.1−0.2 M, 50 °C, MeCN). enclosing 5 demonstrated fairly good activities epoxidation various (3-carene, limonene, α-pinene, cyclohexene, cyclooctene, 1-octene), turnover frequencies (TOF) alkene conversions were close to corresponding parameters achieved homogeneous PWx. For substrates aromatic groups (styrene, cis- trans-stilbenes), a higher level olefin conversion attained using PW12/MIL-101. Moreo...

参考文章(94)
J.-M. Brégeault, R. Thouvenot, S. Zoughebi, L Salles, A. Atlamsani, E. Duprey, C. Aubry, F. Robert, G. Chottard, Novel tungsten catalysts grafted onto polymeric materials: a comparison with phase transfer catalysis Studies in Surface Science and Catalysis. ,vol. 82, pp. 571- 581 ,(1994) , 10.1016/S0167-2991(08)63450-3
J. Mrowiec-Białoń, W. Turek, A.B. Jarzębski, Preparation of highly active heteropolyacid: Silica composite catalysts using the sol-gel method Reaction Kinetics and Catalysis Letters. ,vol. 76, pp. 213- 219 ,(2002) , 10.1023/A:1016515407161
Giorgio Strukul, Catalytic oxidations with hydrogen peroxide as oxidant Kluwer Academic Publishers. ,(1992) , 10.1007/978-94-017-0984-2
Bert F Sels, Aida L Villa, Dirk Hoegaerts, Dirk E De Vos, Pierre A Jacobs, None, Application of heterogenized oxidation catalysts to reactions of terpenic and other olefins with H2O2 Topics in Catalysis. ,vol. 13, pp. 223- 229 ,(2000) , 10.1023/A:1009046703320
Jung Soo Seo, Dongmok Whang, Hyoyoung Lee, Sung Im Jun, Jinho Oh, Young Jin Jeon, Kimoon Kim, A homochiral metal-organic porous material for enantioselective separation and catalysis Nature. ,vol. 404, pp. 982- 986 ,(2000) , 10.1038/35010088
E Stochmal-Pomarzańska, M Hasik, W Turek, A Proń, Preparation, spectroscopic and catalytic studies of poly(1,4-phenylenemethylidynenitrilo-1,4-phenylenenitrilomethylidyne) protonated with selected heteropolyacids Journal of Molecular Catalysis A: Chemical. ,vol. 114, pp. 267- 275 ,(1996) , 10.1016/S1381-1169(96)00326-3
Frédérique Marme, Gisèle Coudurier, Jacques C Védrine, Acid-type catalytic properties of heteropolyacid H3PW12O40 supported on various porous silica-based materials Microporous and Mesoporous Materials. ,vol. 22, pp. 151- 163 ,(1998) , 10.1016/S1387-1811(98)00089-4