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《Journal of The Chinese Rare Earth Society》 1986-02
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Wu Zhiyun, Zhao ongqing, Jiang Min, Li Kai, Zhang Qiang(Jilin University)  
Fourteen lanthanide elements substituted silicotungstic heteropoly acids (I) used as catalysts in methanol conversion have been prepared. By means of IR, DTA,TGA and XRD techniques, some properties in close relationship with catalytic behavior have been determined. Furthermore, the catalytic activities of the fourteen catalysts mentioned above and that of silicomngstic acid have also been investigated.First, K_13[Ln(SiW_11O_39)_2].H_2O (Ln=lanthanide elements except Pm) were synthesized. Then the corresponding acids were prepared by means of the cation exchange under static state eonditions. The obtained acids were supported on silica of expanding pore respectively. These catalysts were heated for 2 hr at 120℃ before reaction.A continuous flow micro-catalytic apparatus was used. The products were analyzed by gas chromatography.The experimental results indicate that the catalytic properties of the heteropoly acid may be improved when the rare earth elements are introduced into tne anion framework of silicotungstie acid as shown by the following data: the conversion increased from 70% (for H_4SiW_12O_40) to 80~93% [for (I)] under same reaction conditions. However, the product distribution is almost the same. On the other hand, the catalytic activities of (I) are also different from each other. Three of Ln-substituted acids (Ln=La~(3+), Gd~(3+), Lu~(3+)) exhibit the highest catalytic activities. P. KOHEHKO et al. have also noted the similar feature. In this paper, some opssible reasons for the phenomenon have been discussed.
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