Dry reforming of methane with isotopic gas mixture over Ni-based pyrochlore catalyst

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Dry reforming of methane was carried out using isotopic 13CO2 and C18O2 gases over a Ni-based pyrochlore catalyst that was synthesized using the modified Pechini method. In this method, 1 wt% Ni was doped into the La2Zr2O7 pyrochlore structure. The catalyst was characterized by H2-TPR, TPO, and XRD and tested for its methane reforming activity under CO2 dry-reforming reaction conditions.The results of repeated TPR/TPO cycles up to 950 °C showed that the consecutive TPR profiles were nearly identical, indicating that the catalyst was stable at high temperatures, and that the nickel oxidation/reduction processes were reversible. The dry-reforming experimental results using labelled 13CO2 gas showed the syngas production for this material proceeded through the activation of CH4 with O that came from breaking one of the CO bonds of CO2 with the latter reaction (CO2 activation) likely occurring at oxygen vacancies at or near the Ni particle-pyrochlore interface. It was also found that only a small portion of the CO originated from CH4. A variation of the same experimental test, but using 12C18O2, revealed only 12C18O was formed and no 12C16O was detected, ruling out the possibility of reaction with the lattice oxygen in the catalyst structure with this material. Over this catalyst, the activated CH4 appeared to dissociate to elemental carbon on the catalyst surface, which was determined to be the source of carbon from a post reaction TPO of the catalyst that was exposed to the 13CO212CH4 mixture. No carbon deposition appeared to originate from 13CO2.