RESUMO
With increasing expectations for carbon neutrality, dry reforming is anticipated for direct conversion of methane and carbon dioxide: the main components of biogas. We have found that dry reforming of methane in an electric field using a Pt/CeO2 catalyst proceeds with sufficient rapidity even at a low temperature of about 473 K. The effect of the electric field (EF) on dry reforming was investigated using kinetic analysis, in situ DRIFTs, XPS, and DFT calculation. In situ DRIFTs and XPS measurements indicated that the amount of carbonate, which is an adsorbed species of CO2, increased with the application of EF. XPS measurements also confirmed the reduction of CeO2 by the reaction of surface oxygen and CH4. The reaction between CH4 molecules and surface oxygen was promoted at the interface between Pt and CeO2.
RESUMO
Low temperature (<500 K) methane steam reforming in an electric field was investigated over various catalysts. To elucidate the factors governing catalytic activity, activity tests and various characterization methods were conducted over various oxides including CeO2, Nb2O5, and Ta2O5 as supports. Activities of Pd catalysts loaded on these oxides showed the order of CeO2 > Nb2O5 > Ta2O5. Surface proton conductivity has a key role for the activation of methane in an electric field. Proton hopping ability on the oxide surface was estimated using electrochemical impedance measurements. Proton transport ability on the oxide surface at 473 K was in the order of CeO2 > Nb2O5 > Ta2O5. The OH group amounts on the oxide surface were evaluated by measuring pyridine adsorption with and without H2O pretreatment. Results indicate that the surface OH group concentrations on the oxide surface were in the order of CeO2 > Nb2O5 > Ta2O5. These results demonstrate that the surface concentrations of OH groups are related to the proton hopping ability on the oxide surface. The concentrations reflect the catalytic activity of low-temperature methane steam reforming in the electric field.
