催化学报

催化学报 ›› 2010, Vol. 31 ›› Issue (1): 61-67.

• 研究论文 • 上一篇    下一篇

SO42−/ZrO2 上异丁烷重构化反应机理的原位核磁共振研究

张丽, 岳斌, 钱林平, 贺鹤勇   

  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, 先进材料实验室, 上海 200433
  • 收稿日期:2010-01-25 出版日期:2010-01-25 发布日期:2010-01-25

In Situ 13C MAS NMR Study on Reaction Mechanism of Isobutane Rearrange-ment over Sulfated Zirconia

ZHANG Li, YUE Bin*, QIAN Linping, HE Heyong*   

  1. Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, Fudan University, Shanghai 200433, China
  • Received:2010-01-25 Online:2010-01-25 Published:2010-01-25

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摘要： 采用原位魔角旋转固体核磁共振技术研究了 2-13C-异丁烷在 SO42−/ZrO2 上的重构化反应机理, 考察了反应温度和 H2 气氛对反应的影响. 结果表明, 反应初期, 异丁烷在 SO42−/ZrO2 上的重构化反应以单分子机理为主, 之后向双分子机理转变; 反应温度的升高有利于单分子机理向双分子机理的转变; H2 的存在抑制了异丁烷的重构化反应, 特别对其双分子机理的反应有较强的抑制作用.

关键词: 硫酸氧化锆, 核磁共振, 异丁烷, 重构化

Abstract: In situ 13C MAS NMR was employed to study the reaction mechanism of isobutane rearrangement over sulfated zirconia using 2-13C-isobutane as a reactant. The effects of temperature and hydrogen atmosphere on the reaction were investigated. The results showed that the reaction of isobutane proceeded mainly via a monomolecular mechanism in its early stage, and then a bimolecular mechanism became dominant. Increasing temperature also led to the reaction from monomolecular to bimolecular mechanism. In the presence of hydrogen, the reaction of isobutane rearrangement, in particular that through the bimolecular pathway, was significantly inhibited.

Key words: sulfated zirconia, nuclear magnetic resonance, isobutane, skeletal rearrangement