Promoting effect of F- on Sr/La oxide catalysts for the oxidative coupling of methane

被引:25
作者
Long, RQ
Zhou, SQ
Huang, YP
Weng, WZ
Wan, HL
Tsai, KR
机构
[1] XIAMEN UNIV,DEPT CHEM,XIAMEN 361005,PEOPLES R CHINA
[2] XIAMEN UNIV,STATE KEY LAB PHYS CHEM SOLID SURFACE,XIAMEN 361005,PEOPLES R CHINA
基金
中国国家自然科学基金;
关键词
methane oxidative coupling; fluoride; oxygen adspecies; in situ IR spectra;
D O I
10.1016/0926-860X(95)00215-4
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 catalytic performance evaluation results showed that the CH4 conversion, C-2 selectivity and ethylene to ethane ratio were significantly higher over LaF3/SrO and SrF2/La2O3 than those over SrO/La2O3 and the maximum C-2 yields of 18-20% were achieved over the LaF3/SrO and SrF2/La2O3 catalysts at 650-750 degrees C. XRD analysis of the fresh catalysts indicated that, with the addition of LaF3 to SrO and treatment in air at high temperature, anionic and/or cationic exchange between oxides and fluorides lattices took place to some extent, leading to the formation of SrF2 and LaOF. The UV spectra of pyridine adsorption and the temperature-programmed desorption spectra of CO2 adsorption on SrF2/La2O3 and SrO/La2O3 showed that surface of the catalyst containing fluoride was more acidic and less basic than that of the corresponding oxide system. The XPS characterizations of O-2-adsorbed catalysts revealed that the catalysts containing F- were more conducive to the formation of the oxygen species with fewer negative charges. The results of in situ IR characterization of the surface oxygen species at 650 degrees C suggested that O-2(-) might be the active oxygen adspecies for the oxidative coupling of methane reaction.
引用
收藏
页码:269 / 280
页数:12
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