Features of deposit formation from 1,3-butadiene over Pd catalysts

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Abstract

Formation of carbonaceous deposits from 1,3-butadiene has been investigated over a group of Pd catalysts. Hydrogen generated in decomposition of diene at 473-523 K participates in diene hydrogenation, resulting in the formation of n-butenes. XRD measurements have confirmed formation of dissolved carbon (PdCx) phase. DRIFT measurements over 0.06 wt.%Pd/γ-Al2O3 have revealed bands at 1575 and 1464 cm-1, suggesting formation of carboxylate structures. Selectivity of the competitive hydrogenation in 1,3-butadiene and propene mixture, R(BD)/R(Pr) has been measured on "fresh" and poisoned samples. Accumulation of deposits has decreased the R(BD)/R(Pr) ratio. The results have been interpreted by transport hindrance and a greater prevalence of non-selective low coordination sites on the poisoned surface. Measurements over Pd, Cu, Pt and Rh catalysts have shown that the high n-butane selectivity over Pt and Rh is also accompanied with low R(BD)/R(Pr) values, suggesting that thermodynamic and mechanistic factors are not entirely separable.

Original languageEnglish
Pages (from-to)153-163
Number of pages11
JournalReaction Kinetics and Catalysis Letters
Volume68
Issue number1
DOIs
Publication statusPublished - Sep 1999

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Keywords

  • Carbonaceous deposit
  • Competitive hydrogenation
  • Dissolved carbon
  • Transport hindrance

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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