表征固体超强酸性的新方法——正丁烷异构化反应的原位^(13)C MAS NMR谱  

A New Method for Characterization of Solid Superacidity:In situ ^(13)C MAS NMR Study of Butane Isomerization on Catalysts

作　　者：马卓娜[1] 胡军成[1] 范康年[1] 曹勇[1] 贺鹤勇[1] 高滋[1] 

机构地区：[1]复旦大学化学系上海市分子催化和功能材料重点实验室,上海200433

出　　处：《化学学报》2003年第9期1352-1356,共5页Acta Chimica Sinica

基　　金：教育部科学技术重点项目 ;国家杰出青年基金 (No .2 0 0 0 531 0 );国家重点基础发展规划项目 (No.2 0 0 0 7750 7)

摘　　要：室温下SO2 -4/ZrO2 催化剂 (SZ)上13 C标记的正丁烷异构化反应的原位13 CMASNMR谱研究结果表明 :其反应动力学符合Langmuir Hinshelwood一级可逆表面反应动力学公式 ,由该动力学公式计算得到的反应速率常数可以用于衡量固体催化剂的表面超强酸性 .这种新的表征方法显示采用一步 -醇热 -超临界干燥综合技术合成的SZ催化剂不仅比表面和硫酸根含量高 ,而且其超强酸性和异构化反应活性均明显优于常规法合成的催化剂 ,具有良好的应用前景 .In situ 13 C MAS NMR study of 13 C-labeled n -butane isomerization on sulfated zirconia (SZ) catalysts shows that the kinetics of n -butane isomerization on SZ catalyst at ambient temperature are well represented by Langmuir-Hinshelwood equation for a reversible first order surface reaction. The calculated isomerization reaction rate constant can be used as a measure of the solid superacidity of the catalysts. The new characterization method reveals that SZ catalysts synthesized from a combined one pot-alcohol thermal-supercritical fluid drying technique not only have high surface area and high sulfate content but their superacidity and isomerization activity are also much higher than those of the conventional SZ catalysts, which is very desirable from the practical point of view.

关 键 词：表征 固体超强酸 正丁烷 异构化反应 原位 13C MAS NMR 硫酸氧化锆 

分 类 号：O643.3[理学—物理化学]