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Impact of Sn Lewis Acid Sites on the Dehydration of Cyclohexanol

  • Karen A. Resende
  • , Ruixue Zhao
  • , Yue Liu
  • , Eszter Baráth*
  • , Johannes A. Lercher*
  • *此作品的通讯作者

科研成果: 期刊稿件文章同行评审

摘要

The impact of Sn on the concentration and strength of acid sites in Al containing zeolites with MFI topology and their catalytic activity for the dehydration of cyclohexanol in the aqueous phase has been investigated. The materials maintain constant Al concentrations and consequently Bro̷nsted acid site (BAS) concentrations, while exhibiting an increasing concentration of Sn Lewis acid sites (LAS). The presence of water alters LAS(Sn), leading to weak BAS(Sn) that increases the concentration of water in the zeolite micropore, while leaving the rate of dehydration of cyclohexanol unchanged. The TOF increases with the concentration of BAS(Al) in close contact with framework LAS(Sn), referred to as BAS(Pair). The increase in the Arrhenius pre-exponential factor, without affecting the activation barrier (Ea), leads to the hypothesis that the proximity of both sites allows for a later transition state induced by the polarization of the C-O bond, leading in turn to a higher transition entropy.

源语言英语
页(从-至)11741-11748
页数8
期刊ACS Catalysis
14
15
DOI
出版状态已出版 - 2 8月 2024
已对外发布

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