Effects of Oxidation–Reduction and Oxychlorination–Reduction Cycles on Pt–Ge/Al2O3 Catalysts

Autor: Colin H. Rochester, James A. Anderson, Geomar J. Arteaga
Rok vydání: 2000
Předmět:
Zdroj: Journal of Catalysis. 189:195-208
ISSN: 0021-9517
Popis: Two Pt(0.3%)–Ge/Al2O3 catalysts containing 0.15 and 0.45% Ge have been characterized by CO chemisorption and FTIR spectra of adsorbed CO after series of oxidation/reduction and oxychlorination/reduction cycles and have also been used for the catalytic hydroreforming of heptane. Catalysts after oxychlorination contained chloro- and oxychloro-Pt complexes which were responsible for the efficient spreading of Pt over the support surface and hence for the maintenance of a good Pt dispersion after reduction. XRD study of a more highly loaded catalyst gave no evidence for Pt–Ge alloy formation or for Ge0 species. Reduced Cl-containing catalysts contained small clustered arrays of Pt atoms dispersed possibly as mats rather than particles over the GeOx-modified alumina such that all the exposed Pt atoms were influenced by an electron withdrawing effect of both Ge2+ ions and Cl ions. Germanium did not block low-coordination Pt sites but may have partially decorated arrays of high coordination sites. Germanium partially stabilized Pt/Al2O3 against loss of activity through coking. The dominant mutual effect of Ge and Cl in catalysts was a significant loss in hydrogenolysis selectivity, but gains in the selectivities of aromatization, isomerization, and cyclization reactions. The addition of Ge to Pt/Al2O3 did not compromise the availability of Pt adsorption sites and only reduced by a small amount the turnover frequencies for heptane reforming reactions. Good activities were therefore maintained in the absence of Ge0 or alloy formation during catalyst reduction.
Databáze: OpenAIRE