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Structure-deactivation relationship for ZSM-5 catalysts governed by framework defects

机译:ZSM-5催化剂的构架失活关系受骨架缺陷控制

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摘要

Zeolites are well known catalysts for the conversion of methanol to hydrocarbons. By adjusting the synthesis procedure, the activity and deactivation of the ZSM-5 zeolite in the conversion of methanol to gasoline can be varied significantly. We found that internal framework defects are crucial for the deactivation behavior of the ZSM-5 catalysts. Adsorption of pyridine and 2,4,6-collidine shows that the infrared band at 3745 cm~(-1) can be assigned to isolated silanol groups on the external surface and the bands at 3726 and 3700 cm~(-1) to silanol groups inside the zeolite crystals. While the activity is related to the acid site density, the deactivation rate correlates with the measured intensity ratio of the IR bands for internal silanols at 3726 cm~(-1) and for external silanol groups at 3745 cm ~(-1) (I3726/I3745). The activity and deactivation, therefore, depend on a different physical property, which means that they can be varied independently.
机译:沸石是众所周知的用于将甲醇转化为烃的催化剂。通过调整合成步骤,可以显着改变ZSM-5沸石在甲醇转化为汽油中的活性和失活。我们发现内部构架缺陷对于ZSM-5催化剂的失活行为至关重要。吡啶和2,4,6-可力丁的吸附表明,在3745 cm〜(-1)处的红外波段可归属于外表面上孤立的硅烷醇基团,而在3726和3700 cm〜(-1)处的波段属于硅烷醇分子在沸石晶体中。虽然活性与酸性位点密度有关,但失活速率与内部硅烷醇在3726 cm〜(-1)和外部硅烷醇基在3745 cm〜(-1)时IR谱带的强度比值相关(I3726 / I3745)。因此,活性和失活取决于不同的物理性质,这意味着它们可以独立变化。

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