Catalytic partial oxidation of methane to synthesis gas over Ni-CeO2

Citation
Tl. Zhu et M. Flytzani-stephanopoulos, Catalytic partial oxidation of methane to synthesis gas over Ni-CeO2, APP CATAL A, 208(1-2), 2001, pp. 403-417
Citations number
54
Categorie Soggetti
Physical Chemistry/Chemical Physics","Chemical Engineering
Journal title
APPLIED CATALYSIS A-GENERAL
ISSN journal
0926860X → ACNP
Volume
208
Issue
1-2
Year of publication
2001
Pages
403 - 417
Database
ISI
SICI code
0926-860X(20010214)208:1-2<403:CPOOMT>2.0.ZU;2-3
Abstract
The partial oxidation of methane to syngas was studied in this work over Ni -containing ceria catalysts with nickel content of 5, 10 and 20 at.% at atm ospheric pressure. All catalysts, in the as prepared state, showed similar activity and CO selectivity at T greater than or equal to 550 degreesC. Cat alyst pre-reduction was nor required. Reaction mixtures were dilute, contai ning 3 mol% CH4 and 1.5 mol% O-2 Methane conversion and CO selectivity appr oached their respective thermodynamic equilibrium values above 550 degreesC . The H-2/CO ratio was equal to 2 at T > 600 degreesC. In the range 0.54-0. 04 g s/cm(3) (STP), contact time effects were absent in partial oxidation o f methane over the 5 at.% Ni-Ce(La), catalyst. The phase composition, nicke l dispersion and carbon deposition on the catalysts were investigated by va rious characterization techniques, including XRD, STEM/EDS, XPS and TPO ana lyses. The 5 at.% Ni-Ce(La)O, catalyst, comprising highly dispersed nickel oxide in ceria, showed excellent resistance to carbon deposition and stable performance during 100 h-on-stream at 650 degreesC, On the other hand, hig h-content (>10 at.%) nickel in ceria, comprising both dispersed nickel and bulk nickel oxide particles, was unstable even after a much shorter time-on -stream: carbon deposition was clearly the cause of this performance instab ility. (C) 2001 Elsevier Science B.V. All rights reserved.