EFFECT OF SURFACE SPECIES ON ACTIVITY AND SELECTIVITY OF MOO3/SIO2 CATALYSTS IN PARTIAL OXIDATION OF METHANE TO FORMALDEHYDE

被引:55
作者
SMITH, MR [1 ]
ZHANG, L [1 ]
DRISCOLL, SA [1 ]
OZKAN, US [1 ]
机构
[1] OHIO STATE UNIV,DEPT CHEM ENGN,COLUMBUS,OH 43210
关键词
METHANE; FORMALDEHYDE; MOLYBDENUM OXIDE; SILICA; RAMAN SPECTROSCOPY; TPR; XPS;
D O I
10.1007/BF00765197
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
The effect of the nature of surface species on the activity and selectivity Of MoO3/SiO2 catalysts has been investigated for the partial oxidation of methane to formaldehyde. Characterization techniques including BET surface area, ambient and in situ Raman spectroscopy, X-ray photoelectron spectroscopy, and temperature-programmed reduction were used in conjunction with steady-state reaction studies to relate the presence of different surface species to the activity and selectivity of the catalyst. Results of these experiments indicate the presence of a highly dispersed silicomolybdic species with terminal Mo=O sites appearing at lower MoO3 loadings. As the weight loading increases, these sites are transformed into polymolybdate species, forming more Mo-O-Mo bridging sites at the expense of Mo=O sites. At high weight loadings, crystalline MoO3 begins to form. The abundance of the Mo=O sites is believed to affect activity and selectivity in the partial oxidation of methane to formaldehyde.
引用
收藏
页码:1 / 15
页数:15
相关论文
共 30 条
[1]   REACTANT COMPOSITION AND CONCENTRATION EFFECTS IN THE OXIDATION OF METHANE ON SUPPORTED 12-MOLYBDOPHOSPHORIC ACID [J].
AHMED, S ;
MOFFAT, JB .
APPLIED CATALYSIS, 1988, 40 (1-2) :101-118
[2]   THE CONVERSION OF METHANE ON HETEROPOLY OXOMETALATES IN THE PRESENCE OF TETRACHLOROMETHANE [J].
Ahmed, Shamsuddin ;
Moffat, John B. .
CATALYSIS LETTERS, 1988, 1 (05) :141-146
[3]  
BARBAUX Y, 1987, CATAL TODAY, V0001, P00147
[4]   STRUCTURE AND CATALYTIC ACTIVITY OF MOO3.SIO2 SYSTEMS .1. SOLID-STATE PROPERTIES [J].
CASTELLAN, A ;
BART, JCJ ;
VAGHI, A ;
GIORDANO, N .
JOURNAL OF CATALYSIS, 1976, 42 (01) :162-172
[5]  
CORDERO RL, 1991, APPL CATAL, V74, P125
[6]   REMARKABLE SPREADING BEHAVIOR OF MOLYBDENA ON SILICA CATALYSTS - AN INSITU EXAFS-RAMAN STUDY [J].
DEBOER, M ;
VANDILLEN, AJ ;
KONINGSBERGER, DC ;
GEUS, JW ;
VUURMAN, MA ;
WACHS, IE .
CATALYSIS LETTERS, 1991, 11 (02) :227-239
[7]  
DRISCOLL SA, 1993, ACS S SERIES, V523
[8]   STRUCTURAL SPECIFICITY OF MOLYBDENUM TRIOXIDE IN C4 HYDROCARBON OXIDATION [J].
HERNANDEZ, RA ;
OZKAN, US .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1990, 29 (07) :1454-1459
[9]   RAMAN-SPECTRA OF COBALT MOLYBDENUM OXIDE SUPPORTED ON SILICA [J].
JEZIOROWSKI, H ;
KNOZINGER, H ;
GRANGE, P ;
GAJARDO, P .
JOURNAL OF PHYSICAL CHEMISTRY, 1980, 84 (14) :1825-1829
[10]   SELECTIVE OXIDATION OF METHANE OVER VYCOR GLASS, QUARTZ GLASS AND VARIOUS SILICA, MAGNESIA AND ALUMINA SURFACES [J].
KASTANAS, GN ;
TSIGDINOS, GA ;
SCHWANK, J .
APPLIED CATALYSIS, 1988, 44 (1-2) :33-51