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
[21]   PARTIAL OXIDATION OF CH4 TO HCHO OVER A MOO3-SIO2 CATALYST - A KINETIC-STUDY [J].
SPENCER, ND ;
PEREIRA, CJ .
AICHE JOURNAL, 1987, 33 (11) :1808-1812
[22]   V2O5-SIO2-CATALYZED METHANE PARTIAL OXIDATION WITH MOLECULAR-OXYGEN [J].
SPENCER, ND ;
PEREIRA, CJ .
JOURNAL OF CATALYSIS, 1989, 116 (02) :399-406
[23]   PARTIAL OXIDATION OF METHANE TO FORMALDEHYDE BY MEANS OF MOLECULAR-OXYGEN [J].
SPENCER, ND .
JOURNAL OF CATALYSIS, 1988, 109 (01) :187-197
[24]   THE EFFECT OF SODIUM ON THE MOO3-SIO2-CATALYZED PARTIAL OXIDATION OF METHANE [J].
SPENCER, ND ;
PEREIRA, CJ ;
GRASSELLI, RK .
JOURNAL OF CATALYSIS, 1990, 126 (02) :546-554
[25]  
STENCEL JM, 1990, RAMAN SPECTROSCOPY C
[26]   CHARACTERIZATION OF SILICA-SUPPORTED MOLYBDENUM OXIDE AND TUNGSTEN-OXIDE - REDUCIBILITY OF THE OXIDIC STATE VERSUS HYDRODESULFURIZATION ACTIVITY OF THE SULFIDED STATE [J].
THOMAS, R ;
VANOERS, EM ;
DEBEER, VHJ ;
MOULIJN, JA .
JOURNAL OF CATALYSIS, 1983, 84 (02) :275-287
[27]   A RAMAN AND ULTRAVIOLET DIFFUSE REFLECTANCE SPECTROSCOPIC INVESTIGATION OF SILICA-SUPPORTED MOLYBDENUM OXIDE [J].
WILLIAMS, CC ;
EKERDT, JG ;
JEHNG, JM ;
HARDCASTLE, FD ;
TUREK, AM ;
WACHS, IE .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (22) :8781-8791
[28]   PARTIAL OXIDATION OF METHANOL TO FORMALDEHYDE OVER MOLYBDENUM OXIDE ON SILICA [J].
YANG, TJ ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1987, 103 (01) :55-64
[29]   PARTIAL OXIDATION OF METHANE WITH NITROUS-OXIDE OVER V2O5-SIO2 CATALYST [J].
ZHEN, KJ ;
KHAN, MM ;
MAK, CH ;
LEWIS, KB ;
SOMORJAI, GA .
JOURNAL OF CATALYSIS, 1985, 94 (02) :501-507
[30]  
[No title captured]