CO2 methanation has aroused intense attention due to the utilization of renewable hydrogen and the production of methane. However, designing Ni-based catalysts with high activity is still under way. This work deals with series of Zr modified supported Ni catalysts for CO2 methanation to improve CO2 conversion and CH4 selectivity at low temperatures. Characterization of catalysts including XRD, N2 physical adsorption, FT-IR, TEM, H2-TPR, H2-TPD and CO2-TPD were carried out to analyze the physicochemical properties for revealing the structure-activity relationship. The addition of citric acid accompanied with zirconia were found to improve the dispersion of Ni nanoparticles by favoring the formation of nickel silicate species and more Ni-ZrO2 interfaces. Consequently, notable presence of Ni nanoparticles confined in the mesoporous channels of SBA-15. Moreover, incorporation of zirconia with appropriate amount on the SBA-15 was found to facilitate basic sites formation, which resulted in generation of formates as identified by operando FTIR analysis, and enhanced catalytic performance. The optimum catalytic performance was obtained over Ni/ZS0.2-C catalyst (citric acid and zirconia added), achieving CO2 conversion as high as 78.1% and nearly 100% CH4 selectivity at 400 °C. In addition, owing to confinement of SBA-15 and the Ni-Zr interaction, no carbon deposits were detected as operation time prolonged to 50 h, manifesting good stability of Ni/ZS0.2-C catalyst.

Highly dispersed Ni particles confined in SBA-15 modified by ZrO2 for enhanced CO2 methanation activity

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