The effect of sulfur poisoning on methane oxidation over palladium supported on γ-alumina catalysts

The effect of sulfur on deactivation of palladium catalysts for methane oxidation has been investigated in this research. A PdO deactivation mechanism due to sulfur is proposed over the 100–400°C range. H2S induced catalyst poisoning of PdO/γ–Al2O3 is attributed to the formation of aluminum sulfate....

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Bibliographic Details
Published inApplied catalysis. B, Environmental Vol. 18; no. 1-2; pp. 105 - 114
Main Authors Yu, Tai-Chiang, Shaw, Henry
Format Journal Article
LanguageEnglish
Published Amsterdam Elsevier B.V 21.09.1998
Elsevier
Subjects
Catalysis
Catalytic reactions
Chemistry
Deactivation
Exact sciences and technology
General and physical chemistry
Methane oxidation
Pd catalysts
Sulfur poisoning
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
Pd catalysts
Deactivation
Methane oxidation
Sulfur poisoning
Methane
Catalyst poisoning
Catalytic reaction
Hydrogen Sulfides
Hydrocarbon
Thermogravimetry
Transition metal
Palladium
Experimental study
Supported catalyst
Infrared spectrometry
Programmed temperature
Heterogeneous catalysis
Gas chromatography
Oxidation
Kinetics
Sulfur
Platinoid
Alumina
Activation energy
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Summary:The effect of sulfur on deactivation of palladium catalysts for methane oxidation has been investigated in this research. A PdO deactivation mechanism due to sulfur is proposed over the 100–400°C range. H2S induced catalyst poisoning of PdO/γ–Al2O3 is attributed to the formation of aluminum sulfate. Catalyst activity decreases with increasing H2S deposition and increasing temperature from 100 to 400°C. TGA results show that PdO promotes the reaction of H2S with γ-Al2O3. Surface sulfite and sulfate groups are observed by FT-IR on poisoned catalysts and are believed to be the cause of a 25% decrease in BET surface area. Activation energy for methane oxidation of H2S poisoned catalyst decreases due to the formation of Al2(SO4)3 which causes the reaction to change from surface reaction control to pore-diffusion control. H2 treatment at 600°C removes much of the sulfite and sulfate from the surface of poisoned catalysts and regenerates most of the fresh catalyst activity.
ISSN:0926-3373
1873-3883
DOI:10.1016/S0926-3373(98)00031-9