Catalytic Partial Oxidation of CH4 over Ni-substituted Barium Hexaaluminate catalysts
Ba{sub 0.75}Ni{sub y}Al{sub 12-y}O{sub 19-{delta}} (y = 0.2, 0.4, 0.6, 0.8 and 1.0) catalysts were tested for the partial oxidation of CH{sub 4} at temperatures between 200 and 900 C. Temperature programmed reaction results indicate that light-off for the partial oxidation reaction occurred between 665 and 687 C for all catalysts. Isothermal runs performed at 900 C on the catalysts showed stable reaction product concentrations, consistent with equilibrium. Post-reaction analysis of the used catalysts showed that there are two distinct zones in the catalyst bed. In a short leading edge of the bed, the apparently complete consumption of oxygen leads to a catalyst which XANES analysis shows is primarily Ni-substituted into the hexaaluminate phase. In the downstream portion of the bed, Ni is shown to be present as metallic Ni. This corresponds to a reaction sequence in which the oxidation of CH{sub 4} proceeds at the inlet until all oxygen is reacted, followed by the reaction of CO{sub 2} and H{sub 2}O with unreacted CH{sub 4}, and its derivatives, to produce the final syngas mixture. From the change in the unit-cell dimensions with Ni substitution, there is a clear indication that Ni{sup 2+}, which has a larger ionic radius than aluminum, substitutes for Al{sup 3+} in the hexaaluminate lattice in the synthesis process, and there is no restructuring of the bulk hexaaluminate phase after the Ni is removed from the lattice.
- Research Organization:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Organization:
- USDOE SC OFFICE OF SCIENCE (SC)
- DOE Contract Number:
- DE-AC02-98CH10886
- OSTI ID:
- 1042183
- Report Number(s):
- BNL-97861-2012-JA; CATTEA; TRN: US201212%%594
- Journal Information:
- Catalysis Today, Vol. 157, Issue 1-4; ISSN 0920-5861
- Country of Publication:
- United States
- Language:
- English
Similar Records
CH4–CO2 reforming over Ni-substituted barium hexaaluminate catalysts
CH4–CO2 reforming over Ni-substituted barium hexaaluminate catalysts