Low-temperature catalytic conversion of greenhouse gases (CO2 and CH4) to syngas over ceria-magnesia mixed oxide supported nickel catalysts

Abstract

Running dry reforming of methane (DRM) reaction at low-temperature is highly regarded to increase thermal efficiency. However, the process requires a robust catalyst that has a strong ability to activate both CH4 and CO2 as well as strong resistance against deactivation at the reaction conditions. Thus, this paper examines the prospect of DRM reaction at low temperature (400–600 °C) over CeO2–MgO supported Nickel (Ni/CeO2–MgO) catalysts. The catalysts were synthesized and characterized by XRD, N2 adsorption/desorption, FE-SEM, H2-TPR, and TPD-CO2 methods. The results revealed that Ni/CeO2–MgO catalysts possess suitable BET specific surface, pore volume, reducibility and basic sites, typical of heterogeneous catalysts required for DRM reaction. Remarkably, the activity of the catalysts at lower temperature reaction indicates the workability of the catalysts to activate both CH4 and CO2 at 400 °C. Increasing Ni loading and reaction temperature has gradually increased CH4 conversion. 20 wt% Ni/CeO2–MgO catalyst, CH4 conversion reached 17% at 400 °C while at 900 °C it was 97.6% with considerable stability during the time on stream. Whereas, CO2 conversions were 18.4% and 98.9% at 400 °C and 900 °C, respectively. Additionally, a higher CO2 conversion was obtained over the catalysts with 15 wt% Ni content when the temperature was higher than 600 °C. This is because of the balance between a high number of Ni active sites and high basicity. The characterization of the used catalyst by TGA, FE-SEM and Raman Spectroscopy confirmed the presence of amorphous carbon at lower temperature reaction and carbon nanotubes at higher temperature.