Abstract
High thermal stability and oxygen conductivity of pyrochlores makes them a potential catalyst for the dry reforming of methane (DRM). In this study, noble metal (Pt, Ru) substituted Ce2Zr2O7 and Ce2Ti2O7 pyrochlores have been synthesized by modified Pechini method. The effect of variation of dopant concentration and position was examined to achieve strong metal-support interaction. Ce2Zr1.96Pt0.04O7-δ exhibited the best catalytic activity towards DRM and hence, been studied for partial oxidation (POM) and autothermal reforming of methane (ATR). Syngas ratio (H2/CO) was tuned by varying the O2 concentration in the feed. Insights obtained from both ex-situ and in situ characterization were exploited to discern the reaction mechanism. The surface intermediates were examined by DRIFTS on Ce2Zr1.96Pt0.04O7-δ for DRM, POM and ATR. Besides adsorbed CH4 and CO on Pt, the presence of carbonate and formate species were also identified. Thus, a dual-site mechanism via carbonate and formate formation was proposed for DRM over Ce2Zr1.96Pt0.04O7-δ.
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