Oxidative coupling of methane over oxide-supported sodium-manganese catalysts
- Texas A & M Univ., College Station, TX (United States)
The oxidative coupling of methane over Mn/Na{sub 2}WO{sub 4}/SiO{sub 2}, Mn/Na{sub 2}WO{sub 4}/MgO, and NaMnO{sub 4}/MgO catalysts was studied using both a cofeed flow system and a pulse reactor. At 800{degrees}C and 1 atm, and using a CH{sub 4}/O{sub 2} ratio of ca. 8/1, a methane conversion of 20% was achieved at a C{sub 2+} selectivity of {ge}80%, with no diluent in the reagents. The similar catalytic behaviors of the three catalysts suggest that a common active site, consisting of an Na-O-Mn species, may be involved. Results from a pulse reaction sequence (an O{sub 2} pulse followed by a series of pure CH{sub 4} pulses) indicate that the active species are not stable under reaction conditions unless gas phase O{sub 2} is present, and that bulk lattice oxygen does not participate in the methane coupling reaction when carried out in the cofeed mode. There is a linear relationship between the specific activity for CH{sub 4} conversion and the concentration of surface Mn, which is believed to be responsible for the activation of O{sub 2}. The resulting form of oxygen then abstracts a hydrogen atom from CH{sub 4}. Sodium is essential for preventing the complete oxidation of CH{sub 4}, perhaps by isolating the Mn ions. The tungstate ions appear to impart stability to the catalysts. 39 refs., 11 figs., 5 tabs.
- OSTI ID:
- 486297
- Journal Information:
- Journal of Catalysis, Vol. 155, Issue 2; Other Information: PBD: 1 Sep 1995
- Country of Publication:
- United States
- Language:
- English
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