EXAFS and activity studies of the poisoning effect on Cl on Pt/Al{sub 2}O{sub 3} catalysts during oxidation reactions.
The effect of Cl on the activity of Pt/Al{sub 2}O{sub 3} catalysts for methane oxidation has been studied by H{sub 2} and CO chemisorption, O{sub 2} isotopic exchange, kinetic studies and EXAFS spectroscopy. Catalysts containing 1.5% pt/Al{sub 2}O{sub 3} were prepared by incipient wetness from H{sub 2}PtCl{sub 6} and Pt(NH{sub 3}){sub 4}(NO{sub 3}){sub 2} precursors. Both reduced catalysts have similar dispersion (0.8) as determined by H{sub 2} chemisorption. At low methane concentration (0.3 vol.% CH{sub 4}, 16 vol.% O{sub 2}) the Cl-free catalyst was about 20 times more active during complete methane oxidation than the Cl-containing catalyst. Both CO chemisorption and oxygen exchange were observed on the Cl-free catalyst, whereas they were not detected on the Cl-containing catalyst. On the Cl-free catalyst, only Pt-Pt and Pt-O bonds were detected from the EXAFS results, while on the Cl-containing catalyst additional Pt-Cl bonds were present. The effect of chlorine on activity strongly depended on the reactant concentration. Exposure of the Cl-free catalyst to higher concentrations of methane (3 vol.% CH{sub 4}) reduced the activity to a level similar to that of the Cl-containing catalyst. Addition of HCl to the Cl-free catalyst rendered the activity identical to the catalyst prepared from Cl-containing precursors. A model is proposed to explain the mechanism of chloride poisoning, which appears to be site blocking.
- Research Organization:
- Argonne National Lab., IL (US)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- W-31-109-ENG-38
- OSTI ID:
- 799780
- Report Number(s):
- ANL/CMT/CP-104452; TRN: US200224%%250
- Resource Relation:
- Conference: 9th International Symposium on Catalyst Deactivation (9th ISCD), Lexington, KY (US), 10/07/2001--10/10/2001; Other Information: PBD: 5 Apr 2001
- Country of Publication:
- United States
- Language:
- English
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