化学学报 ›› 2003, Vol. 61 ›› Issue (9): 1352-1356. 上一篇    下一篇

研究论文

表征固体超强酸性的新方法-正丁烷异构化反应的原位~(13)CMASNMR谱

马卓娜;胡军成;范康年;曹勇;贺鹤勇;高滋   

  1. 复旦大学化学系
  • 发布日期:2003-09-15

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

Ma Zhuona;Hu Juncheng;Fan Kangnnian;Cao Yong;He Heyong;Gao Zi   

  1. Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University
  • Published:2003-09-15

室温下SO_4~(2-)/ZrO_2催化剂(SZ)上~(13)C标记的丁烷异构化反应的原位 ~(13)C MAS NMR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。

关键词: 氧化锆, 丁烷, 异构化, 超强酸, 碳13核磁共振谱法, 硫酸, 反应动力学

In situ ~(13)C MAS NMR study of ~(13)C-labeled n-butane isomerization on sulfated zirnmia (SZ) ralalysLs shows that the kinetics of n-butane isomerization on SZ catalyst at ambient temperature arc well mpmsented by Langmuir-Hinshelwood equation for a reversible first order surface reaction. The calculated isranerizatinn reaction rate constant can be used as a measure of the solid superacidity of the catalysts. The new characterization method iwi'iil. H 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 isomeiization activity are also much higher than those of the conventional SZ catalysts, which is very desirable from the practical point of view.

Key words: ZIRCONIUM OXIDE, BUTANE, ISOMERIZATION, SUPERACID, C13NMR, SULFURIC ACID

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