Self-poisoning and aging of Pd-Ag/Al2O3 in semi-hydrogenation of 1,3-butadiene: Effects of surface inhomogeneity caused by hydrocarbonaceous deposits

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Abstract

Effects of hydrocarbonaceous deposits have been investigated in hydrogenation of 1,3-butadiene over Pd-Ag/Al2O3 catalysts. Studies on the effect of various treatments on self-poisoned samples revealed very different behavior of the surface deposits. Because of hydrogen's low surface fugacity, hydrogen treatment was not sufficient to remove surface species at T<373 K. Vacuum or O2 treatment increased the activity of the self-poisoned samples. The observation has been interpreted in terms of surface restructuring of the firmly held species. Deliberate poisoning - amount of deposits 1-20 mg/gcat - increased the selectivity of n-butane formation. Presence of deposits seems to decrease the effective surface concentration of butadiene. The results have been interpreted as slow diene transport allowing saturation of n-butenes on a certain fraction of sites.

Original languageEnglish
Pages (from-to)111-118
Number of pages8
JournalStudies in Surface Science and Catalysis
Volume111
DOIs
Publication statusPublished - Jan 1 1997

ASJC Scopus subject areas

  • Catalysis
  • Condensed Matter Physics
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

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