4.6 Article

TAP study of toluene total oxidation over a Co3O4/La-CeO2 catalyst with an application as a washcoat of cordierite honeycomb monoliths

期刊

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 16, 期 23, 页码 11447-11455

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c4cp00886c

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资金

  1. Long Term Structural Methusalem - Flemish Government
  2. Ministry of Science and Innovation of Spain/FEDER Program of the EU [MAT2008-00889/NAN]
  3. Junta de Andalucia [FQM-110]

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The total oxidation of toluene was studied over a Co3O4/La-CeO2 catalyst in a Temporal Analysis of Products (TAP) set-up in the temperature range 713 K to 873 K in the presence and absence of dioxygen. It has been demonstrated that the reaction proceeds via a Mars-van Krevelen mechanism. The reaction rate increased 8.4 times if both toluene and dioxygen were present in the feed. The partial reaction order with respect to O-2 diminished from 0.9 to 0.6 with an increase in temperature from 763 to 873 K. Adsorbed oxygen species with a lifetime of similar to 8 s have been found on a catalyst fully oxidized by dioxygen. Catalysis of isotopically labeled O-18(2)/(C6H5CH3)-C-12-C-13 results in the formation of products containing O-18, which indicates that both lattice and adsorbed oxygen are involved in the total oxidation of toluene. The role of adsorbed oxygen is activation of the C-H bond in toluene. The reaction network of the catalytic total oxidation of toluene consists of the following sequence: adsorption of toluene on the catalyst surface; activation of toluene by dehydrogenation with adsorbed oxygen; oxidation of activated toluene mainly by the lattice oxygen and re-oxidation of the reduced catalyst by dioxygen.

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