Correlations between Dispersion, Acidity, Reducibility, and Propane Aromatization Activity of Gallium Species Supported on HZSM5 Zeolites

被引:85
作者
Rodrigues, Victor de O. [1 ]
Eon, Jean-Guillaume [1 ]
Faro, Arnaldo C., Jr. [1 ]
机构
[1] Univ Fed Rio de Janeiro, Inst Quim, Rio De Janeiro, Brazil
关键词
CHEMICAL-VAPOR-DEPOSITION; DEHYDROGENATION REACTION; H-ZSM5; CATALYSTS; OXIDE; ACTIVATION; ALKANES; ZSM-5; STATE; IONS; DEHYDROCYCLIZATION;
D O I
10.1021/jp910642p
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Gallium-modified ZSM5 zeolites, containing 2, 3, and 4 wt % Ga, were prepared by incipient wetness impregnation with gallium(111) nitrate Solutions of HZSM5 samples with SAR values of 24 and 35. The modified zeolites were Subjected to two consecutive treatment cycles of reduction in hydrogen and reoxidation in air. The catalysts were characterized by nitrogen physical adsorption, Si-29 and Al-27 MAS NMR, temperature-programmed reduction, temperature-programmed desorption of ammonia, X-ray absorption spectroscopy, and infrared spectroscopy in the OH stretching region and in the region of skeletal vibrations of adsorbed pyridine. Catalytic activity and selectivity were measured ill propane conversion reactions at 703 K. Results were rationalized in terms of correlations among the framework Ga/Al ratio, density, strength and type of acidity, gallium Cluster sizes, reducibility of gallium. and propane aromatization activity. It Was found that the dispersion of the gallium Species Was a function only of the Framework Ga/Al ratio. Lewis acidity and reducibility of the gallium species were positively correlated with each other and with their degree of dispersion. A correlation Was Found between propane aromatization activity and the product of the concentrations of strong Lewis and Bronsted acid sites in the oxide form of the catalysts.
引用
收藏
页码:4557 / 4567
页数:11
相关论文
共 41 条
[1]   A reinvestigation of beta-gallium oxide [J].
Ahman, J ;
Svensson, G ;
Albertsson, J .
ACTA CRYSTALLOGRAPHICA SECTION C-CRYSTAL STRUCTURE COMMUNICATIONS, 1996, 52 :1336-1338
[2]   Preparation of gallium-containing catalysts by solid-state reaction of acidic Zeolites with elemental gallium [J].
Altwasser, S ;
Raichle, A ;
Traa, Y ;
Weitkamp, J .
CHEMICAL ENGINEERING & TECHNOLOGY, 2004, 27 (12) :1262-1265
[3]   Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure [J].
Ankudinov, AL ;
Ravel, B ;
Rehr, JJ ;
Conradson, SD .
PHYSICAL REVIEW B, 1998, 58 (12) :7565-7576
[4]   NATURE OF THE ACTIVE-SITES IN H-ZSM-11 ZEOLITE MODIFIED WITH ZN(2+) AND GA(3+) [J].
ANUNZIATA, OA ;
PIERELLA, LB .
CATALYSIS LETTERS, 1993, 19 (2-3) :143-151
[5]  
Areán CO, 2001, PHYS CHEM CHEM PHYS, V3, P1223
[6]   Structure and function of metal cations in light alkane reactions catalyzed by modified H-ZSM5 [J].
Biscardi, JA ;
Iglesia, E .
CATALYSIS TODAY, 1996, 31 (3-4) :207-231
[7]   SYNTHESIS AND CHARACTERIZATION OF GALLOSILICATES AND GALLOALUMINOSILICATES ISOMORPHOUS TO ZEOLITE-BETA [J].
CAMBLOR, MA ;
PEREZPARIENTE, J ;
FORNES, V .
ZEOLITES, 1992, 12 (03) :280-286
[8]   Gallium-containing zeolites: characterization of catalytic role of gallium species in converting light paraffins to aromatics [J].
Chao, KJ ;
Liu, PH .
CATALYSIS SURVEYS FROM ASIA, 2005, 9 (01) :11-15
[9]   X-ray absorption spectroscopic study on the states of gallium and platinum in Pt/Ga/H-beta zeolites [J].
Chao, KJ ;
Wei, AC ;
Wu, HC ;
Lee, JF .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 35-6 :413-424
[10]   Influence of Si/Ga and Si/Al ratios on propane aromatization over highly active H-GaAlMFI [J].
Choudhary, TV ;
Kinage, A ;
Banerjee, S ;
Choudhary, VR .
CATALYSIS COMMUNICATIONS, 2006, 7 (03) :166-169