Abstract
The kinetics of CO2reforming of CH4were studied over Pt supported on TiO2, ZrO2, Cr2O3, and SiO2, and the catalysts were characterized using chemisorption, X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), temperature-programmed hydrogenation (TPH), and temperature-programmed surface reaction. Although the Pt/SiO2and Pt/Cr2O3catalysts deactivated significantly within 5 and 15 h onstream, respectively, the Pt/ZrO2and Pt/TiO2catalysts exhibited much higher stability even after 80 to 100 h onstream. TPH results with used catalysts showed that both Pt/ZrO2and Pt/TiO2have suppressed carbon deposition under reaction conditions. H2and CO chemisorption as well as DRIFTS provided evidence of metal–support interactions in the Pt/TiO2catalyst and indicated that large ensembles of Pt atoms, active for carbon deposition, are deactivated or destroyed by the presence of mobile TiOxspecies. Activities for CO formation and CH4consumption on a turnover frequency basis were five times greater on Pt/TiO2compared with the other catalysts, suggesting that active sites for reforming are created in the Pt–TiOxinterfacial region. The kinetic behavior was explained well by a kinetic model recently proposed for supported Ni.
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