Catalytic oxidative dehydrogenation of propane over Mg-V/Mo oxides

被引:70
作者
Pless, JD
Bardin, BB
Kim, HS
Ko, DG
Smith, MT
Hammond, RR
Stair, PC
Poeppelmeier, KR
机构
[1] Northwestern Univ, Dept Chem, Inst Environm Catalysis, Evanston, IL 60208 USA
[2] Dow Chem Co USA, S Charleston, WV 25303 USA
[3] Rubicon Technol Inc, Ctr Res & Dev, Deerfield, IL 60015 USA
基金
美国国家科学基金会;
关键词
propane; oxidative dehydrogenation; ODH; magnesium; vanadium; and molybdenum oxides; Raman spectroscopy;
D O I
10.1016/j.jcat.2004.01.023
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
Fifteen distinct MgO-V2O5, MgO-MoO3, MgO-V2O5-MoO3, and V2O5-MOO3 compositions were prepared using sol-gel chemistry and their selectivities and conversions for propane oxidative dehydrogenation (ODH) to propylene were measured. The vanadates were more active than the molybdates at lower temperatures; however, the molybdates exhibited higher selectivities at similar conversions. An increase in both ODH conversion and selectivity with molybdenum substitution on vanadium sites was also observed. These results demonstrate the importance of the bulk structure on the ODH reaction. In general, propylene selectivities increased with increasing conversions at temperatures above 673 K when oxygen depletion in the reactant stream occurred. Visible and UV Raman spectroscopy corroborates this result and helps focus attention on critical surface-specific information. A new Raman peak was observed for the partially reduced MgMoO4 and is associated with a three-coordinate surface oxygen. (C) 2004 Elsevier Inc. All rights reserved.
引用
收藏
页码:419 / 431
页数:13
相关论文
共 89 条
[1]   Oxidative dehydrogenation of of propane over molybdenum supported on MgO-gamma-Al2O3 [J].
Abello, MC ;
Gomez, MF ;
Cadus, LE .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1996, 35 (07) :2137-2143
[2]   Key aspects of catalyst design for the selective oxidation of paraffins [J].
Albonetti, S ;
Cavani, F ;
Trifiro, F .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1996, 38 (04) :413-438
[3]   Preparation and characterization of rare earth orthovanadates for propane oxidative dehydrogenation [J].
Au, CT ;
Zhang, WD ;
Wan, HL .
CATALYSIS LETTERS, 1996, 37 (3-4) :241-246
[4]   Molecular structures of supported metal oxide catalysts under different environments [J].
Bañares, MA ;
Wachs, IE .
JOURNAL OF RAMAN SPECTROSCOPY, 2002, 33 (05) :359-380
[5]   VIBRATIONAL-SPECTRUM OF MAGNESIUM ORTHOVANADATE [J].
BARAN, EJ .
MONATSHEFTE FUR CHEMIE, 1975, 106 (01) :1-11
[6]   On the partial oxidation of propane and propylene on mixed metal oxide catalysts [J].
Bettahar, MM ;
Costentin, G ;
Savary, L ;
Lavalley, JC .
APPLIED CATALYSIS A-GENERAL, 1996, 145 (1-2) :1-48
[7]   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
[8]   Quantitative determination of the number of surface active sites and the turnover frequency for methanol oxidation over bulk metal vanadates [J].
Briand, LE ;
Jehng, JM ;
Cornaglia, L ;
Hirt, AM ;
Wachs, IE .
CATALYSIS TODAY, 2003, 78 (1-4) :257-268
[9]   SPECTROSCOPIC CHARACTERIZATION OF MAGNESIUM VANADATE CATALYSTS .1. VIBRATIONAL CHARACTERIZATION OF MG3(VO4)2,MG2V2O7 AND MGV2O6 POWDERS [J].
BUSCA, G ;
RICCHIARDI, G ;
SAM, DSH ;
VOLTA, JC .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1994, 90 (08) :1161-1170
[10]   Oxidative dehydrogenation of propane over Mg-Mo-O catalysts [J].
Cadus, LE ;
Abello, MC ;
Gomez, MF ;
Rivarola, JB .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1996, 35 (01) :14-18