Kinetic regimes in the tandem reactions of H-BEA catalyzed formation of p-xylene from dimethylfuran [electronic resource]

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Ngôn ngữ: eng

Ký hiệu phân loại: 666.6 Earthenware and stoneware

Thông tin xuất bản: Washington, D.C. : Oak Ridge, Tenn. : United States. Dept. of Energy. Office of Science ; Distributed by the Office of Scientific and Technical Information, U.S. Dept. of Energy, 2015

Mô tả vật lý: Size: p. 178-187 : , digital, PDF file.

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ID: 263580

 Reaction kinetics and pathways of p-xylene formation from 2,5-dimethylfuran (DMF) and ethylene via cascade reactions of Diels?Alder cycloaddition and subsequent dehydration over H-BEA zeolite (Si/Al = 12.5) were characterized. Two distinct kinetic regimes were discovered corresponding to the rate limiting reaction, namely Diels?Alder cycloaddition and cycloadduct dehydration, as the concentration of Br�nsted acid sites decreases. At catalyst loadings with effective acid site concentrations exceeding a critical value (~2.0 mM), the rate of formation of Diels?Alder products becomes constant. Under these conditions, the measured activation energy of 17.7 � 1.4 kcal mol<
 sup>
 -1<
 /sup>
  and reaction orders correspond to the [4 + 2] Diels?Alder cycloaddition reaction of DMF and ethylene. Conversely, at catalyst loadings below the critical value, the formation rate of p-xylene becomes first order in catalyst loading, and the measured activation energy of 11.3 � 3.5 kcal mol<
 sup>
 -1<
 /sup>
  is consistent with dehydration of the Diels?Alder cycloadduct to p-xylene. Experimental comparison between H-BEA and H-Y zeolite catalysts at identical conditions indicates that the micropore structure controls side reactions such as furan dimerization and hydrolysis
  the latter is supported via molecular simulation revealing a substantially higher loading of DMF within H-Y than within H-BEA zeolites at reaction conditions.
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