Insight into the active site nature of zeolite H-BEA for liquid phase etherification of isobutylene with ethanol

作者: Nina V. Vlasenko , Yuri N. Kochkin , German M. Telbiz , Oleksiy V. Shvets , Peter E. Strizhak

DOI: 10.1039/C9RA07721A

关键词:

摘要: The nature of active acid sites zeolite H-BEA with different Si/Al ratios (15–407) in liquid phase etherification isobutylene ethanol a continuous flow reactor the temperature range 80–180 °C has been explored. We describe and discuss data concerning strength concentration obtained by techniques stepwise (quasi-equilibrium) thermal desorption ammonia, X-ray diffraction, low-temperature adsorption nitrogen, FTIR spectroscopy adsorbed pyridine solid-state 27Al MAS NMR. average values energy NH3 on were experimentally determined as 63.7; 91.3 121.9 mmol g−1 (weak, medium, strong, respectively). In agreement this, correlation between rate ethyl-tert-butyl ether synthesis weak (ENH3 = 61.6–68.9 kJ mol−1) observed. It was concluded that for this reaction are Bronsted hydroxyls representing internal silanol groups associated octahedrally coordinated aluminum second coordination sphere.

参考文章(111)
M. Hunger, T. Horvath, Sorption of methanol on zeolite HBeta investigated by in situ MAS NMR spectroscopy Catalysis Letters. ,vol. 49, pp. 95- 100 ,(1997) , 10.1023/A:1019028532141
Mario G. Clerici, Zeolites for fine chemicals production Topics in Catalysis. ,vol. 13, pp. 373- 386 ,(2000) , 10.1023/A:1009063106954
G. Busca, M. Bevilacqua, T. Armaroli, M. Trombetta, FT-IR studies of internal, external and extraframework sites of FER, MFI, BEA and MOR type protonic zeolite materials Studies in Surface Science and Catalysis. ,vol. 142, pp. 975- 982 ,(2002) , 10.1016/S0167-2991(02)80126-4
Ramón Alcántara, Elena Alcántara, Laureano Canoira, María José Franco, Ismael Martín, Alberto Navarro, Gas-Phase Synthesis of Ethyl tert-Butyl Ether (ETBE) on H-ZSM-5 Catalyst in Continuous Fixed-Bed and Fluidized-Bed Reactors Reaction Kinetics and Catalysis Letters. ,vol. 69, pp. 239- 246 ,(2000) , 10.1023/A:1005631313062
Vasiliĭ Nikolaevich Tikhonov, Analytical chemistry of Aluminum ,(1973)
G. Bellussi, P. Pollesel, Industrial applications of zeolite catalysis: production and uses of light olefins Studies in Surface Science and Catalysis. ,vol. 158, pp. 1201- 1212 ,(2005) , 10.1016/S0167-2991(05)80466-5
S. Altwasser, J. Jiao, S. Steuernagel, J. Weitkamp, M. Hunger, Elucidating the dealumination mechanism of zeolite H-Y by solid-state NMR spectroscopy Studies in Surface Science and Catalysis. ,vol. 154, pp. 1212- 1213 ,(2004) , 10.1016/S0167-2991(04)80630-X
Silvia Bordiga, Carlo Lamberti, Francesca Bonino, Arnaud Travert, Frédéric Thibault-Starzyk, Probing zeolites by vibrational spectroscopies Chemical Society Reviews. ,vol. 44, pp. 7262- 7341 ,(2015) , 10.1039/C5CS00396B