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A series of Ni-xSi/ZrO2 (x = 0, 0.1, 0.5, 1 wt%, the controlled contents of Si) catalysts with a controlled nickel content of 10 wt% were prepared by the co-impregnation method with ZrO2 as support and Si as a promoter. The effect of different amounts of Si on the catalytic performance was investigated for CO2 methanation with the stoichiometric H2/CO2 molar ratio (4/1). The catalysts were characterized by BET, XRF, H2-TPR, H2-TPD, H2-chemisorption, CO2-TPD, XRD, TEM, XPS, and TG-DSC. It was found that adding the appropriate amount of Si could improve the catalytic performance of Ni/ZrO2 catalyst at a low reaction temperature (250 °C). Among all the catalysts studied, the Ni-0.1Si/ZrO2 catalyst showed the highest catalytic activity, with H2 and CO2 conversion of 73.4% and 72.5%, respectively and the yield of CH4 was 72.2%. Meanwhile, the catalyst showed high stability and no deactivation within a 10 h test. Adding the appropriate amount of Si could enhance the interaction between Ni and ZrO2, and increase the Ni dispersion, the amounts of active sites including surface Ni0, oxygen vacancies, and strong basic sites on the catalyst surface. These might be the reasons for the high activity and selectivity of the Ni-0.1Si/ZrO2 catalyst. [ABSTRACT FROM AUTHOR]