Abstract: Large surface areas nano-scale zirconia was prepared by the self-assembly route and was employed as support in nickel catalysts for the CO selective methanation. The effects of Ni loading and the catalyst calcination temperature on the performance of the catalyst for CO selective methanation reaction were investigated. The catalysts were characterized by Brunauer-Emmett-Teller (BET), transmission electron microscope (TEM), X-ray diffraction (XRD) and temperature-programmed reduction (TPR). The results showed that the as-synthesized Ni/nano-ZrO₂ catalysts presented high activity for CO methanation due to the interaction between Ni active particle and nano zirconia support. The selectivity for the CO methanation influenced significantly by the particle size of the active Ni species. The exorbitant calcination resulted in the conglomeration of dispersive Ni particles and led to the decrease of CO methanation selectivity. Among the catalysts studied, the 7.5% (by mass) Ni/ZrO₂ catalyst calcinated at 500℃ was the most effective for the CO selective methanation. It can preferentially catalyze the CO methanation with a higher 99% conversion in the CO/CO₂ competitive methanation system over the temperature range of 260-280℃, while keeping the CO₂ conversion relatively low.

Key words: selective CO methanation, CO removal, nano zirconia, Ni catalysts

摘要： Large surface areas nano-scale zirconia was prepared by the self-assembly route and was employed as support in nickel catalysts for the CO selective methanation. The effects of Ni loading and the catalyst calcination temperature on the performance of the catalyst for CO selective methanation reaction were investigated. The catalysts were characterized by Brunauer-Emmett-Teller (BET), transmission electron microscope (TEM), X-ray diffraction (XRD) and temperature-programmed reduction (TPR). The results showed that the as-synthesized Ni/nano-ZrO₂ catalysts presented high activity for CO methanation due to the interaction between Ni active particle and nano zirconia support. The selectivity for the CO methanation influenced significantly by the particle size of the active Ni species. The exorbitant calcination resulted in the conglomeration of dispersive Ni particles and led to the decrease of CO methanation selectivity. Among the catalysts studied, the 7.5% (by mass) Ni/ZrO₂ catalyst calcinated at 500℃ was the most effective for the CO selective methanation. It can preferentially catalyze the CO methanation with a higher 99% conversion in the CO/CO₂ competitive methanation system over the temperature range of 260-280℃, while keeping the CO₂ conversion relatively low.

关键词: selective CO methanation, CO removal, nano zirconia, Ni catalysts