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- Title
Isotopic Studies on the Mechanism of Partial Oxidation of CH4 to Syngas over a Ni/Al2O3 Catalyst.
- Authors
Li, Chunyi; Yu, Changchun; Shen, Shikong
- Abstract
An isotopic transient technique and XPS were used to investigate the mechanism of partial oxidation of CH4 to syngas over a Ni/Al2O3 catalyst at atmospheric pressure and 700°C. The experimental results show that CH4 can decompose easily and quickly to H2 and Ni xC over the reduced catalyst, and Ni xC can react rapidly with NiO from Ni oxidized by O2 to CO or CO2 depending on the relative concentration of Ni xC around NiO on the catalyst surface. Both H2 and CO are primary products in partial oxidation of CH4. Isotopic tracing experiments prove that most of CO2 produced during partial oxidation of CH4 is from the surface reaction between Ni xC and NiO, and it is impossible to mainly originate from the further oxidation of CO or the disproportionation of CO. The disproportionation of CO may happen at the experimental conditions, limited by thermodynamic equilibrium, however, the conversion of CO is very low. The pulse experiments of CH4/O2 and CH4/CO2 with stoichiometric ratio show that the rate of partial oxidation of CH4 is faster than that of CH4 reforming with CO2, this implies that partial oxidation of CH4 is unlikely to proceed via a combustion reforming mechanism. All the results support the direct oxidation mechanism: H2 is from CH4 decomposition and CO is the product of the surface reaction between Ni xC and NiO.
- Publication
Catalysis Letters, 2001, Vol 75, Issue 3/4, p183
- ISSN
1011-372X
- Publication type
Article
- DOI
10.1023/A:1016744005805