Influence of carbon-oxygen surface complexes on the surface acidity of tungsten oxide catalysts supported on activated carbons

被引:38
作者
Moreno-Castilla, C [1 ]
Pérez-Cadenas, AF
Maldonado-Hódar, FJ
Carrasco-Marín, F
Fierro, JLG
机构
[1] Univ Granada, Fac Ciencias, Dept Quim Inorgan, Granada 18071, Spain
[2] CSIC, Inst Catalisis & Petr Quim, Madrid 28049, Spain
关键词
activated carbon; catalyst support; surface oxygen complexes;
D O I
10.1016/S0008-6223(03)00023-X
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
Tungsten oxide catalysts supported on activated carbons were prepared by using tungsten hexacarbonyl, ammonium tungstate. and tungsten pentaethoxide as precursors. An activated carbon was obtained from olive stone by physical activation. A portion of this activated carbon was oxidized with ammonium peroxydisulfate in order to introduce different oxygen surface complexes. Subsequently, different portions of this oxidized activated carbon were heat treated in nitrogen flow at various temperatures to partially remove the oxygen surface complexes. In this way, activated carbons with different amounts of oxygen surface complexes were obtained, which were then used as supports for the tungsten oxide catalysts. Both the supports and the supported catalysts were pre-treated either in He, dry air or wet air flow at 623 K for 6 h. They were then characterized by X-ray photoelectron spectroscopy, X-ray diffraction, measurements of the pH of the point of zero charge, and activity in the decomposition reaction of isopropanol. Turnover frequencies for the formation of propene were obtained. According to these results, the oxygen surface complexes of the support have a major influence on the total acidity of the tungsten oxide supported catalysts. In some supported catalysts, W(VI) was reduced to W(V) during the decomposition reaction of isopropanot as a consequence of the hydrogen evolution. The results indicate that oxygen surface complexes of the support may play an important role in this reduction process, which was inhibited when the support had high surface oxygen content. (C) 2003 Elsevier Science Ltd. All rights reserved.
引用
收藏
页码:1157 / 1167
页数:11
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