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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

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【作者】 李涛王胜高典楠王树东

【Author】 LI Tao;WANG Sheng;GAO Dian-nan;WANG Shu-dong;Dalian National Laboratory for Clean Energy (DNL) ,Dalian Institute of Chemical Physics ,Chinese Academy of Sciences;University of Chinese Academy of Sciences;

【机构】 中国科学院大连化学物理研究所洁净能源国家实验室中国科学院大学

【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10000 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Ru Cl3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-1and H2/CO2 mol ratio of 3.5.

  • 【文献出处】 燃料化学学报 ,Journal of Fuel Chemistry and Technology , 编辑部邮箱 ,2014年12期
  • 【分类号】O643.32
  • 【被引频次】9
  • 【下载频次】193
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