制备条件对Ru/Ce0.8Zr0.2O2催化剂上CO2甲烷化反应性能的影响

Effect of support calcination temperature on the catalytic properties of Ru/Ce0.8Zr0.2O2 for methanation of carbon dioxide

    摘要
  • 摘要: 采用均相法制得Ce0.8Zr0.2O2载体,并以其为载体等体积浸渍制得一系列负载型Ru催化剂。在0.1 MPa、GHSV为10 000 h-1、H2/CO2为3.5(物质的量比)的条件下,对催化剂进行评价。借助TG-DSC、BET、H2-TPR等技术对所制备的载体和催化剂进行表征,结果表明,500 ℃焙烧的载体具有适中的比表面积和孔径并形成了Ce-Zr固溶体,与载体形成弱相互作用的Ru能够显著提高催化剂的活性,适宜的还原方式能促进活性组分的均匀分布。采用500 ℃焙烧的载体浸渍RuCl3溶液,干燥后在400 ℃焙烧,并使用水合肼和H2两次还原后的催化剂活性最高,在290 ℃时,H2转化率可达到93.57%。

     

    Abstract: A series of Ru/Ce0.8Zr0.2O2 catalysts were prepared by the impregnation method with Ce0.8Zr0.2O2 homoprecipitated and calcined at different temperatures as supports. The supports and the catalysts were characterized with TG-DSC, BET and H2-TPR techniques. It was shown that the Ce0.8Zr0.2O2 calcined at 500 ℃ formed Ce-Zr solid solution and had a proper surface area and pore opening and a weak interaction with Ru species, leading to a significant increase in the catalytic activity. A suitable reduction methods promoted distribution of active species. The Ru/Ce0.8Zr0.2O2 prepared with the Ce0.8Zr0.2O2 calcined at 500 ℃ showed high activity after calcination at 400 ℃ and successive reduction with H2N·NH2·H2O and H2. It gave a H2 conversion of 93.57%, approaching to the equilibrium value under the conditions of 290 ℃, 0.1 MPa, 10 000 h-1 and H2/CO2 mol ratio of 3.5.

     

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