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高比表面钛铌复合氧化物在气相Beckmann重排反应中的催化应用
Catalytic Application of Titanoniobium Composite Oxides with a High Specific Surface Area in the Vapor-Phase Beckmann Rearrangement
【摘要】 以K2CO3、Nb2O5和TiO2为原料,经高温固相反应制得KTiNbO5,进一步与HCl溶液反应后得到HTiNbO5。HTiNbO5经用长链有机胺预支撑,再与含Ti(IV)聚合阳离子溶液反应,所得产物在空气气氛中焙烧后制备出高比表面钛铌复合氧化物。它是一类多孔材料,其BET比表面积达80~100 m2.g-1。测试了该复合氧化物以及在该复合氧化物上负载B2O3后所得担载型催化剂在环己酮肟气相贝克曼重排反应中的催化性能。当B2O3负载量为7.31%(质量分数)时,环己酮肟转化率(~100%)在4.5 h内无明显改变,反应进行6 h后,转化率仍高于85%;己内酰胺选择性接近或超过90%且在整个反应过程中基本不变。
【Abstract】 KTiNbO5 was synthesized by heating a stoichiometric mixture of K2CO3,La2O3,and Nb2O5,and HTiNbO5 was obtained by ion exchange of KTiNbO5 in HCl solution.HTiNbO5 was pre-expanded by long-chain alkylamine,then reacting with a solution containing Ti(IV) polycations,followed by calcining the obtained precursor in air,two titanoniobium composite oxides(designated as HTNO) with a high specific surface area were prepared.The products were porous materials,and their BET surface areas were 80 ~ 100 m2·g-1.The vapor phase Beckmann rearrangement reaction of cyclohexanone oxime was studied with HTNO and B2O3/HTNO as catalysts.The B2O3/HTNO catalyst with B2O3 loading of 7.31 wt % exhibited 100% conversion of the oxime with ε-caprolactam selectivity near or beyond 90%.The conversion was no significant change within 4.5 h and still higher than 85% after 6 h.
【Key words】 titanoniobium composite oxide; high specilic surface area; catalytic application; vapor phase Beckmann rearrangement reaction;
- 【文献出处】 天然气化工 ,Natural Gas Chemical Industry , 编辑部邮箱 ,2006年01期
- 【分类号】O643.32
- 【被引频次】7
- 【下载频次】227