Impact of Sn Lewis Acid Sites on the Dehydration of Cyclohexanol

Sn路易斯酸位对环己醇脱水的影响

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作者:Karen A Resende, Ruixue Zhao, Yue Liu, Eszter Baráth, Johannes A Lercher

Abstract

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 (E a), 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.

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