Investigating the Effect of Ni Loading on the Performance of Yttria-Stabilised Zirconia Supported Ni Catalyst during CO2 Methanation

Abstract

CO2 methanation was studied on Ni-based yttria-stabilised zirconia (Ni/YSZ) catalysts. The catalysts were prepared by the wet impregnation method, where the amount of Ni content was varied from 5% to 75%. Thereafter, the prepared catalysts were analysed by BET, XRD, SEM and H2-TPR. BET results showed an initial increase in the surface area with an increase in Ni loading, then a decrease after 30% Ni loading. The XRD results revealed that the Ni crystallite size increased as the Ni loading increased, while the H2-TPR showed a shift in reduction peak temperature to a higher temperature, indicating that the reducibility of the catalysts decreased as the Ni loading increased. The activity of the synthesised catalysts for CO2 methanation was studied by passing a mixture of H2, CO2 and N2 with a total flow of 135 mL min−1 and GHSV of 40,500 mL h−1 g−1 through a continuous flow quartz tube fixed-bed reactor (I.D. = 5.5 mm, wall thickness = 2 mm) containing 200 mg of the catalyst at a temperature range of 473 to 703 K under atmospheric pressure and a H2:CO2 ratio of 4. The tested Ni/YSZ catalysts showed an improvement in activity as the reaction temperature increased from 473 K to around 613 to 653 K, depending on the Ni loading. Beyond the optimum temperature, the catalyst’s activity started to decline, irrespective of the Ni loading. In particular, the 40% Ni/YSZ catalyst displayed the best performance, followed by the 30% Ni/YSZ catalyst. The improved activity at high Ni loading (40% Ni) was attributed to the increase in hydrogen coverage and improved site for both H2 and CO2 adsorption and activation.