V2O5-SiO2 systems prepared by flame pyrolysis as catalysts for the oxidative dehydrogenation of propane

被引:65
作者
Rossetti, I. [1 ]
Fabbrini, L. [1 ]
Ballarini, N. [2 ]
Oliva, C. [1 ]
Cavani, F. [2 ]
Cericola, A. [2 ]
Bonelli, B. [3 ]
Piumetti, M. [3 ]
Garrone, E. [3 ]
Dyrbeck, H. [4 ]
Blekkan, E. A. [4 ]
Forni, L. [1 ]
机构
[1] Univ Milan, CNR, Dipartimento CFE & ISTM, I-20133 Milan, Italy
[2] Univ Bologna, Dipartimento Chim Ind & Mat, INSTM, Res Unit Bologna,NoE Idecat Partner FP6 EU, I-40126 Bologna, Italy
[3] Politecn Torino, Dipartimento Sci Mat & Ingn Chim, INSTM Unit, Turin, Italy
[4] Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway
关键词
propane ODH; flame pyrolysis; silica-supported vanadium; anaerobic and co-feed reaction conditions;
D O I
10.1016/j.jcat.2008.02.028
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
VOx/SiO2 catalysts were prepared through an innovative flame pyrolysis (FP) technique and tested for the oxidative dehydrogenation of propane. The samples, of different V loadings, were characterized by electron paramagnetic resonance (EPR), micro-Raman, and FT-IR spectroscopy to assess the nature of the vanadium active sites in comparison with a sample prepared by impregnation. The active sites of the FP-prepared catalysts appeared as highly dispersed V5+O groups partly incorporated into the silica matrix and interacting poorly with one another. Lower dispersion can be achieved at the same V loading with the catalyst prepared by impregnation. EPR revealed V4+O groups pointing out normally from the catalyst surface and sitting in the center of a surface array of oxygen atoms. These V4+ groups helped demonstrate the difference in catalytic behavior of the various samples. Catalytic activity measured under both aerobic and anaerobic conditions revealed a promisingly high selectivity with the FP-prepared samples. The best results were obtained with a 10 wt% V loading, which provided the best propylene yield among the samples, especially under anaerobic conditions (up to 80% selectivity at 10% propane conversion). This is likely related to the much higher dispersion of the VOx species in the FP-prepared samples, which also helps reduce the coke formation triggered by exposed surface acid sites. (C) 2008 Elsevier Inc. All rights reserved.
引用
收藏
页码:45 / 61
页数:17
相关论文
共 55 条
[1]   Extent of reduction of vanadium oxides during catalytic oxidation of alkanes measured by in-situ UV-visible spectroscopy [J].
Argyle, MD ;
Chen, KD ;
Resini, C ;
Krebs, C ;
Bell, AT ;
Iglesia, E .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (07) :2345-2353
[2]   Effect of catalyst structure on oxidative dehydrogenation of ethane and propane on alumina-supported vanadia [J].
Argyle, MD ;
Chen, KD ;
Bell, AT ;
Iglesia, E .
JOURNAL OF CATALYSIS, 2002, 208 (01) :139-149
[3]   The oxygen-assisted transformation of propane to COx/H2 through combined oxidation and WGS reactions catalyzed by vanadium oxide-based catalysts [J].
Ballarini, N. ;
Battisti, A. ;
Cavani, F. ;
Cericola, A. ;
Lucarelli, C. ;
Racioppi, S. ;
Arpentinier, P. .
CATALYSIS TODAY, 2006, 116 (03) :313-323
[4]   Supported vanadium oxide-based catalysts for the oxidehydrogenation of propane under cyclic conditions [J].
Ballarini, N ;
Cavani, F ;
Cericola, A ;
Cortelli, C ;
Ferrari, M ;
Trifirò, F ;
Capannelli, G ;
Comite, A ;
Catani, R ;
Cornaro, U .
CATALYSIS TODAY, 2004, 91-2 :99-104
[5]   Oxydehydrogenation of propane catalyzed by V-Si-O cogels: enhancement of the selectivity to propylene by operation under cyclic conditions [J].
Ballarini, N ;
Cavani, F ;
Ferrari, M ;
Catani, R ;
Cornaro, U .
JOURNAL OF CATALYSIS, 2003, 213 (01) :95-102
[6]   The combination of propane partial oxidation and of WGS reaction in a single catalytic bed, and the self-adapting catalytic properties of vanadium oxide catalyst [J].
Ballarini, Nicola ;
Battisti, Andrea ;
Cavani, Fabrizio ;
Cericola, Antonio ;
Cortelli, Carlotta ;
Ferrari, Maria ;
Trifiro, Feffuccio ;
Arpentinier, Philippe .
APPLIED CATALYSIS A-GENERAL, 2006, 307 (01) :148-155
[7]   Oxidative dehydrogenation of ethane and n-butane on VOx/Al2O3 catalysts [J].
Blasco, T ;
Galli, A ;
Nieto, JML ;
Trifiro, F .
JOURNAL OF CATALYSIS, 1997, 169 (01) :203-211
[8]   Oxidative dehydrogenation of short chain alkanes on supported vanadium oxide catalysts [J].
Blasco, T ;
Nieto, JML .
APPLIED CATALYSIS A-GENERAL, 1997, 157 (1-2) :117-142
[9]   Kinetic investigations on the oxidehydrogenation of propane over vanadium supported on γ-Al2O3 [J].
Bottino, A ;
Capannelli, G ;
Comite, A ;
Storace, S ;
Di Felice, R .
CHEMICAL ENGINEERING JOURNAL, 2003, 94 (01) :11-18
[10]  
BURNEAU A, 1999, SURFACE PROPERTIES S, P194