Electrochemical Promotion of Nanostructured Palladium Catalyst for Complete Methane Oxidation

Abstract

Electrochemical promotion of catalysis (EPOC) was investigated for methane complete oxidation over palladium nano-structured catalysts deposited on yttria-stabilized zirconia (YSZ) solid electrolyte. The catalytic rate was evaluated at different temperatures (400, 425 and 450 °C), reactant ratios and polarization values. The electrophobic behavior of the catalyst, i.e., reaction rate increase upon anodic polarization was observed for all temperatures and gas compositions with an apparent Faradaic efficiency as high as 3000 (a current application as low as 1 μA) and maximum rate enhancement ratio up to 2.7. Temperature increase resulted in higher enhancement ratios under closed-circuit conditions. Electrochemical promotion experiments showed persistent behavior, where the catalyst remained in the promoted state upon current or potential interruption for a long period of time. An increase in the polarization time resulted in a longer-lasting persistent promotion (p-EPOC) and required more time for the reaction rate to reach its initial open-circuit value. This was attributed to continuous promotion by the stored oxygen in palladium oxide, which was formed during the anodic polarization in agreement with p-EPOC mechanism reported earlier.