INVESTIGATIONS OF ACTIVE-SITES FOR METHANE ACTIVATION IN THE OXIDATIVE COUPLING REACTION OVER PURE AND LI-PROMOTED MGO CATALYSTS

被引:64
作者
WU, MC [1 ]
TRUONG, CM [1 ]
COULTER, K [1 ]
GOODMAN, DW [1 ]
机构
[1] TEXAS A&M UNIV SYST,DEPT CHEM,COLL STN,TX 77843
关键词
D O I
10.1006/jcat.1993.1089
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 oxidative coupling of methane to ethane over model MgO catalysts prepared under well-controlled, ultrahigh vacuum (UHV) conditions has been studied using a combination of surface science techniques and elevated-pressure kinetic measurements. The utilization of electron energy loss spectroscopy has allowed us to characterize a variety of defects and to identify the active sites which are responsible for the methane coupling reaction. The results indicate that [Li+O-] centers are not likely directly involved in the methane activation step, but rather promote the production of F-type centers in the near-surface region which are responsible for this key step in the methane coupling reaction. The origin of [Li+O-] and F-type defects and their densities and stabilities are discussed. © 1993 Academic Press, Inc.
引用
收藏
页码:344 / 352
页数:9
相关论文
共 32 条
[21]   OXIDATIVE COUPLING OF METHANE TO HIGHER HYDROCARBONS [J].
LEE, JS ;
OYAMA, ST .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1988, 30 (02) :249-280
[22]  
Lunsford J.H., 1990, CATAL TODAY, V6, P235
[23]   OXIDATIVE COUPLING OF METHANE OVER LITHIUM-DOPED ULTRAFINE CRYSTALLINE MAGNESIUM-OXIDE [J].
MATSUURA, I ;
UTSUMI, Y ;
DOI, T ;
YOSHIDA, Y .
APPLIED CATALYSIS, 1989, 47 (02) :299-306
[24]   A MODEL FOR THE OXIDATION OF MG(0001) BASED UPON LEED, AES, ELS AND WORK FUNCTION MEASUREMENTS [J].
NAMBA, H ;
DARVILLE, J ;
GILLES, JM .
SURFACE SCIENCE, 1981, 108 (03) :446-482
[25]   THERMALLY GENERATED [LI]0 CENTERS IN CAO [J].
OLSON, DN ;
ORERA, VM ;
CHEN, Y ;
ABRAHAM, MM .
PHYSICAL REVIEW B, 1980, 21 (03) :1258-1263
[26]   SURFACE-COMPOSITION AND REACTIVITY OF LITHIUM-DOPED MAGNESIUM-OXIDE CATALYSTS FOR OXIDATIVE COUPLING OF METHANE [J].
PENG, XD ;
RICHARDS, DA ;
STAIR, PC .
JOURNAL OF CATALYSIS, 1990, 121 (01) :99-109
[27]   ELECTRONIC SPECTRUM AND ULTRAVIOLET OPTICAL PROPERTIES OF CRYSTALLINE MG0 [J].
ROESSLER, DM ;
WALKER, WC .
PHYSICAL REVIEW, 1967, 159 (03) :733-&
[28]   CHARACTERIZATION OF [LI+O-] CENTERS IN LITHIUM-DOPED MGO CATALYSTS [J].
WANG, JX ;
LUNSFORD, JH .
JOURNAL OF PHYSICAL CHEMISTRY, 1986, 90 (22) :5883-5887
[29]  
WEBER H, 1951, Z PHYS, V30, P392
[30]   ELECTRON-ENERGY-LOSS-SPECTROSCOPY STUDIES OF THERMALLY GENERATED DEFECTS IN PURE AND LITHIUM-DOPED MGO(100) FILMS ON MO(100) [J].
WU, MC ;
TRUONG, CM ;
GOODMAN, DW .
PHYSICAL REVIEW B, 1992, 46 (19) :12688-12694