Support effect in dehydrogenation of propane in the presence Of CO2 over supported gallium oxide catalysts

被引:206
作者
Xu, BJ
Zheng, B
Hua, WM [1 ]
Yue, YH
Gao, Z
机构
[1] Fudan Univ, Dept Chem, Shanghai 200433, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200433, Peoples R China
基金
中国国家自然科学基金; 上海市自然科学基金;
关键词
supported gallium oxide catalyst; propane; dehydrogenation; carbon dioxide; reaction mechanism;
D O I
10.1016/j.jcat.2006.02.017
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
Dehydrogenation of propane to propene in the absence or presence of CO2 over different supported gallium oxide catalysts was investigated. Ga2O3/TiO2, Ga2O3/AbO(3), and Ga2O3/ZrO2 catalysts exhibited high activity, and Ga2O3/SiO2 and Ga2O3/MgO were ineffective catalysts for the dehydrogenation of propane. The conversions of propane over Ga2O3/TiO2, Ga2O3/Al2O3. and Ga2O3/ZrO2 catalysts at 600 degrees C reached 23, 33, and 39%, respectively. The high dehydrogenation activities are connected with the abundant medium-strong acid sites on the catalyst surface. Carbon dioxide can promote the catalytic dehydrogenation activity of Ga2O3/TiO2 but suppress those of Ga2O3/ZrO2 and Ga2O3/Al2O3. The conversion of propane becomes 32, 26, and 30% in the presence of CO2 over Ga2O3/TiO2. Ga2O3/Al2O3, and Ga2O3/ZrO2 catalysts. respectively. Results of pulse reaction and the H-2 and propane chemisorptions indicate that two contrary roles of CO2 exist in the reaction: the positive role of removing dissociatively adsorbed H-2 on catalyst surface through the reverse water-gas shift reaction and the negative role of displacing the propane adsorbed on basic sites of catalyst. XPS studies show that the different behavior of the five supported Ga2O3 catalysts may be attributed to the different interactions between the support and the Ga2O3 species. The dehydrogenation reaction is suggested to proceed through a heterolytic dissociation reaction pathway. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:470 / 477
页数:8
相关论文
共 27 条
[1]   LOW-TEMPERATURE REDUCTION OF GALLIUM IN A GA2O3 HZSM-5 CATALYST [J].
CARLI, R ;
BIANCHI, CL ;
GIANNANTONIO, R ;
RAGAINI, V .
JOURNAL OF MOLECULAR CATALYSIS, 1993, 83 (03) :379-389
[2]   Study of reverse water gas shift reaction by TPD, TPR and CO2 hydrogenation over potassium-promoted Cu/SiO2 catalyst [J].
Chen, CS ;
Cheng, WH ;
Lin, SS .
APPLIED CATALYSIS A-GENERAL, 2003, 238 (01) :55-67
[3]   Hydrogen chemisorption on gallium oxide polymorphs [J].
Collins, SE ;
Baltanás, MA ;
Bonivardi, AL .
LANGMUIR, 2005, 21 (03) :962-970
[4]   Gallium-hydrogen bond formation on gallium and gallium-palladium silica-supported catalysts [J].
Collins, SE ;
Baltanás, MA ;
Fierro, JLG ;
Bonivardi, AL .
JOURNAL OF CATALYSIS, 2002, 211 (01) :252-264
[5]   AROMATIZATION OF SHORT CHAIN ALKANES ON ZEOLITE CATALYSTS [J].
GUISNET, M ;
GNEP, NS ;
ALARIO, F .
APPLIED CATALYSIS A-GENERAL, 1992, 89 (01) :1-30
[6]   Ga2O3/Al2O3 prepared by sol-gel method as a highly active metal oxide-based catalyst for NO reduction by propene in the presence of oxygen, H2O and SO2 [J].
Haneda, M ;
Kintaichi, Y ;
Shimada, H ;
Hamada, H .
CHEMISTRY LETTERS, 1998, (02) :181-182
[7]   EFFECT OF GA/PROTON BALANCE IN GA/HZSM-5 CATALYSTS ON C-3 CONVERSION TO AROMATICS [J].
KWAK, BS ;
SACHTLER, WMH .
JOURNAL OF CATALYSIS, 1994, 145 (02) :456-463
[8]   Gallium based MFI zeolites for the aromatization of propane [J].
Meriaudeau, P ;
Naccache, C .
CATALYSIS TODAY, 1996, 31 (3-4) :265-273
[9]   DEHYDROGENATION AND DEHYDROCYCLIZATION CATALYTIC PROPERTIES OF GALLIUM OXIDE [J].
MERIAUDEAU, P ;
NACCACHE, C .
JOURNAL OF MOLECULAR CATALYSIS, 1989, 50 (01) :L7-L10
[10]   THE ROLE OF GA2O3 AND PROTON ACIDITY ON THE DEHYDROGENATING ACTIVITY OF GA2O3-HZSM-5 CATALYSTS - EVIDENCE OF A BIFUNCTIONAL MECHANISM [J].
MERIAUDEAU, P ;
NACCACHE, C .
JOURNAL OF MOLECULAR CATALYSIS, 1990, 59 (03) :L31-L36