CO2 Methanation over Hydrotalcite-Derived Nickel/Ruthenium and Supported Ruthenium Catalysts

Abstract

In this work, in-house synthesized NiMgAl, Ru/NiMgAl, and Ru/SiO2 catalysts and a commercial ruthenium-containing material (Ru/Al2O3com.) were tested for CO2 methanation at 250, 300, and 350 °C (weight hourly space velocity, WHSV, of 2400 mLN,CO2·g−1·h−1). Materials were compared in terms of CO2 conversion and CH4 selectivity. Still, their performances were assessed in a short stability test (24 h) performed at 350 °C. All catalysts were characterized by temperature programmed reduction (TPR), X-ray diffraction (XRD), N2 physisorption at −196 °C, inductively coupled plasma optical emission spectrometry (ICP-OES), and H2/CO chemisorption. The catalysts with the best performance (i.e., the hydrotalcite-derived NiMgAl and Ru/NiMgAl) seem to be quite promising, even when compared with other methanation catalysts reported in the literature. Extended stability experiments (240 h of time-on-stream) were performed only over NiMgAl, which was selected based on catalytic performance and estimated price criteria. This catalyst showed some deactivation under conditions that favor CO formation (high temperature and high WHSV, i.e., 350 °C and 24,000 mLN,CO2·g−1·h−1, respectively), but at 300 °C and low WHSV, excellent activity (ca. 90% of CO2 conversion) and stability, with nearly complete selectivity towards methane, were obtained.