Syngas production from partial oxidation of methane over Ce1-XNiXOY catalysts prepared by complexation-combustion method

Synthesis gas production from partial oxidation of methane (CH4/O2/Ar = 4/2/94) over Ce1−XNiXOY (X = 0.05–0.6) catalysts was investigated between 500 and 900 °C by using a jet stirred reactor. The highest conversion rate of CH4 and O2 was obtained on Ce0.6Ni0.4OY where the selectivity of hydrogen wa...

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Veröffentlicht in:Applied catalysis. A, General General, 2006-09, Vol.311, p.24-33
Hauptverfasser: WENJUAN SHAN, FLEYS, Matthieu, LAPICQUE, Francois, SWIERCZYNSKI, Dariusz, KIENNEMANN, Alain, SIMON, Yves, MARQUAIRE, Paul-Marie
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Sprache:eng
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Zusammenfassung:Synthesis gas production from partial oxidation of methane (CH4/O2/Ar = 4/2/94) over Ce1−XNiXOY (X = 0.05–0.6) catalysts was investigated between 500 and 900 °C by using a jet stirred reactor. The highest conversion rate of CH4 and O2 was obtained on Ce0.6Ni0.4OY where the selectivity of hydrogen was close to 80% and the CO selectivity was higher than 90%, although the residence time was very low (δ = 3 s). The desired ratio H2/CO about 2 was obtained at about 700 °C for all catalysts. Moreover, the catalyst exhibited good stability as no reaction activity decrease was observed during 160 h reaction at 650 °C due to the high redox property of the catalyst in the reaction. The structure and property of the catalysts were investigated by XRD, TPR, BET, N2-adsorption, and XPS for the fresh and used samples. The TPR and XPS results suggested that Ce3+/Ce4+ and Ni2+/Ni0 couples coexisted in the reaction by Ni2+ + Ce3+ + □ → Ni0 + Ce4+ due to the strong interaction between the Ni and Ce species in the catalysts. The lattice oxygen actived by Ce3+ with oxygen vacancy is the main active oxygen species for the reaction. Both Ni0 and Ce3+ with oxygen vacancy are the active sites for the reaction. The active site transferred between Ni0 and Ce3+-□ depending on the availability of lattice oxygen in the reaction.
ISSN:0926-860X
1873-3875
DOI:10.1016/j.apcata.2006.05.044