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Citation: He He-Yong, Zou Yan, Ma Zhuo-Na, Yue Bin. In situ MAS NMR Spectroscopy Study on Catalytic Reaction Mechanism of Light Alkanes[J]. Acta Physico-Chimica Sinica, ;2004, 20(08S): 1024-1031. doi: 10.3866/PKU.WHXB200408zk20 shu

In situ MAS NMR Spectroscopy Study on Catalytic Reaction Mechanism of Light Alkanes

1.
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai　200433

Received Date: 16 February 2004
Available Online: 15 August 2004

In situ MAS NMR spectroscopy has been successfully applied to study catalytic reaction mechanisms. Examples taken from our own study illustrate that the batch-like condition in situ MAS NMR technique with strategically 13C labeled reactants can contribute to the understanding of reaction pathway. The results indicate that the ion-exchanged and/or its related Ga species are the highly active catalytic components for the activation of propane under mild condition over Ga-modified H-MFI catalysts. Reaction mechanism of skeletal isomerization of n-butane over a series of solid acid catalysts in the acidic strength order of SO42-/ZrO2, CsxH3－xPW12O40 and H-MOR was also studied. The mechanism of n-butane isomerization is dependent on the type of solid acid catalyst. Under low temperature, n-butane isomerization on SO42-/ZrO2 and CsxH3－xPW12O40 catalysts proceeds through a monomolecular pathway in the initial stage of the reaction. At the later stage, C3 and C5 are detected, giving the evidence of the contribution of the bimolecular process. On H-MOR catalyst, n-butane isomerization occurs primarily via a bimolecular pathway. Further study shows that the kinetics of n-butane isomerization on SO42-/ZrO2 catalyst at ambient temperature can be 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.
- In situ;Solid state NMR;Mechanism;Catalytic reaction;Light alkanes
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