Dry Reforming of Methane Using Rh Substituted Pyrochlores

Accelerating Fossil Energy Technology Development Through Integrated Computation and Experimentation
AIChE Annual Meeting
October 31, 2012 - 1:15pm-1:30pm
Dry (CO2) reforming of methane (DRM) to syngas (H2 and CO) has been well-studied over a number of catalysts. The high temperatures needed to produce syngas inevitably result in carbon formation. Although pyrochlores are known to be thermally stable at conditions required for dry reforming, we are aware of only one reference in which DRM has been studied (Ashcroft et al., 1993) over pyrochlores. The potential for substituted pyrochlores to exhibit both thermally stability and to resist carbon formation due to their inherent oxygen conductivity suggest that they may be active and stable for DRM. Here, we report the use of Rh-substituted- lanthanum zirconate (La2Zr2O7) pyrochlores for DRM. Isomorphic substitution of Rh as the active metal on the B-site results in an active and stable catalyst for DRM. Specifically three catalysts (a) unsubstituted lanthanum zirconate (LZ) for baseline comparison, (b) 2% and (c) 5% (by wt) Rh-substituted L2RhZ and L5RhZ pyrochlores were characterized using CH4 and H2 temperature programmed reduction (TPR) and their activity was studied at different temperatures of 550 ºC, 575 ºC, and 600 ºC. H2 TPR showed that the reducibility of the pyrochlore increases with an increase in the metal substitution. CH4 TPR clearly shows that the lattice oxygen in pyrochlores is reactive and helps limit carbon formation. Activity results showed that the CH4 and CO2 conversion increase with an increase in metallic substitution into the pyrochlore lattice.
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