H2 Production from Catalytic Methane Decomposition Using Fe/x-ZrO2 and Fe-Ni/(x-ZrO2) (x = 0, La2O3, WO3) Catalysts

Abstract

An environmentally-benign way of producing hydrogen is methane decomposition. This study focused on methane decomposition using Fe and Fe-Ni catalysts, which were dispersed over different supports by the wet-impregnation method. We observed the effect of modifying ZrO2 with La2O3 and WO3 in terms of H2 yield and carbon deposits. The modification led to a higher H2 yield in all cases and WO3-modified support gave the highest yield of about 90% and was stable throughout the reaction period. The reaction conditions were at 1 atm, 800 °C, and 4000 mL(hgcat)−1 space velocity. Adding Ni to Fe/x-ZrO2 gave a higher H2 yield and stability for ZrO2 and La2O3 + ZrO2-supported catalysts whose prior performances and stabilities were very poor. Catalyst samples were analyzed by characterization techniques like X-ray diffraction (XRD), nitrogen physisorption, temperature-programmed reduction (TPR), thermo-gravimetric analysis (TGA), and Raman spectroscopy. The phases of iron and the supports were identified using XRD while the BET revealed a significant decrease in the specific surface areas of fresh catalysts relative to supports. A progressive change in Fe’s oxidation state from Fe3+ to Fe0 was observed from the H2-TPR results. The carbon deposits on Fe/ZrO2 and Fe/La2O3 + ZrO2 are mainly amorphous, while Fe/WO3 + ZrO2 and Fe-Ni/x-ZrO2 are characterized by graphitic carbon.