Direct observation of hexamethylbenzenium radical cations generated during zeolite methanol-to-olefin catalysis: an ESR study.
作者： Sun Jung Kim , Hoi-Gu Jang , Jun Kyu Lee , Hyung-Ki Min , Suk Bong Hong
DOI: 10.1039/C1CC13153B
关键词: Methanol 、 Direct observation 、 Reaction intermediate 、 Olefin fiber 、 Molecular sieve 、 Spectroscopy 、 Catalysis 、 Zeolite 、 Photochemistry 、 Chemistry
摘要: The generation of hexamethylbenzenium radical cations as the key reaction intermediate in chabazite-type molecular sieve acids (i.e., H-SAPO-34 and H-SSZ-13) during methanol-to-olefin process has been directly evidenced by ESR spectroscopy.
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postech.ac.kr参考文章(37)
Weiguo Song, John B. Nicholas, Alain Sassi, James F. Haw, Synthesis of the Heptamethylbenzenium Cation in Zeolite-β: in situ NMR and Theory Catalysis Letters. ,vol. 81, pp. 49- 53 ,(2002) , 10.1023/A:1016003905167
A.V. Kucherov, A.A. Slinkin, D.A. Kondratyev, T.N. Bondarenko, A.M. Rubinstein, Kh.M. Minachev, Formation of radicals and catalytic activity of H-ZSM-5-type zeolites in unsaturated hydrocarbon conversions: Part 2. Radical formation upon adsorption of aromatic compounds Journal of Molecular Catalysis. ,vol. 37, pp. 107- 115 ,(1986) , 10.1016/0304-5102(86)85141-0
Bjørnar Arstad, Stein Kolboe, Ole Swang, Theoretical study of the heptamethylbenzenium ion. Intramolecular isomerizations and C2, C3, C4 alkene elimination. Journal of Physical Chemistry A. ,vol. 109, pp. 8914- 8922 ,(2005) , 10.1021/JP058166F
James F. Haw, John B. Nicholas, Weiguo Song, Feng Deng, Zhike Wang, Teng Xu, Catherine S. Heneghan, Roles for Cyclopentenyl Cations in the Synthesis of Hydrocarbons from Methanol on Zeolite Catalyst HZSM-5 Journal of the American Chemical Society. ,vol. 122, pp. 4763- 4775 ,(2000) , 10.1021/JA994103X
Kwang Young Lee, Ho-Jeong Chae, Soon-Yong Jeong, Gon Seo, None, Effect of crystallite size of SAPO-34 catalysts on their induction period and deactivation in methanol-to-olefin reactions Applied Catalysis A-general. ,vol. 369, pp. 60- 66 ,(2009) , 10.1016/J.APCATA.2009.08.033
Morten Bjørgen, Unni Olsbye, Dirk Petersen, Stein Kolboe, The methanol-to-hydrocarbons reaction: insight into the reaction mechanism from [12C]benzene and [13C]methanol coreactions over zeolite H-beta Journal of Catalysis. ,vol. 221, pp. 1- 10 ,(2004) , 10.1016/S0021-9517(03)00284-7
Ivar M. Dahl, Stein Kolboe, On the Reaction Mechanism for Hydrocarbon Formation from Methanol over SAPO-34 Journal of Catalysis. ,vol. 161, pp. 304- 309 ,(1996) , 10.1006/JCAT.1996.0188
A. F. Bedilo, A. M. Volodin, G. A. Zenkovets, G. V. Timoshok, Formation of cation radicals from methylbenzenes on sulfated zirconia Reaction Kinetics and Catalysis Letters. ,vol. 55, pp. 183- 190 ,(1995) , 10.1007/BF02075849
Weiguo Song, Hui Fu, James F. Haw, Supramolecular origins of product selectivity for methanol-to-olefin catalysis on HSAPO-34. Journal of the American Chemical Society. ,vol. 123, pp. 4749- 4754 ,(2001) , 10.1021/JA0041167
Morten Bjørgen, Finn Joensen, Karl-Petter Lillerud, Unni Olsbye, Stian Svelle, The mechanisms of ethene and propene formation from methanol over high silica H-ZSM-5 and H-beta Catalysis Today. ,vol. 142, pp. 90- 97 ,(2009) , 10.1016/J.CATTOD.2009.01.015