迟亚武,梁东白,徐长海,林培滋,罗洪原,林励吾.预处理条件对用于CO_2加氢的超细CuO-ZnO-SiO_2催化剂性能的影响[J].分子催化,1996,(6):
预处理条件对用于CO_2加氢的超细CuO-ZnO-SiO_2催化剂性能的影响
Effect of Pretreatment Conditions on the Properties and Activities of Ultrafine CuO ZnO SiO 2 Catalysts for Hydrogenation of Carbon Dioxide
  
DOI:
中文关键词:  焙烧温度,还原温度,超细催化剂,CO2加氢,CuO-ZnO-SiO2
英文关键词:Calcination temperature, Reduction temperature, Ultra fine catalyst, Hydrogenation of carbon dioxide, CuO ZnO SiO 2
基金项目:
迟亚武  梁东白  徐长海  林培滋  罗洪原  林励吾
中国科学院大连化学物理研究所
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中文摘要:
      采用XRD、BET、TPR手段,研究了焙烧和还原温度对超细CuO-ZnO-SiO2催化剂的性质及其CO2加氢反应催化活性的影响.胶体在573-773K范围内焙烧生成CuO、Cu2O、ZnO晶相,随着焙烧温度继续升高,CuO和ZnO晶粒逐渐变大,但催化剂的比表面积和孔容变化很小.在973K焙烧后出现Zn2SiO4晶相,使催化剂比表积和孔容变小,导致催化剂活性降低.焙烧温度对催化剂活性的影响大于对CO2加氢产物分布的影响.在548-648K范围内,催化剂还原温度对其催化活性影响不大.703K高温还原后,可能由于Cu0晶粒的出现,使得催化剂的活性下降.TPR研究结果进一步表明,焙烧温度影响CuO同ZnO、SiO2之间的相互作用和催化剂的还原行为.
英文摘要:
      The effects of ruduction and calcination temperature on the properties and activities of ultrafine CuO ZnO SiO 2 catalysts prepared by sol gel method for hydrogenation of carbon dioxide were investigated by XRD, BET and TPR techniques. When calcination temperatures were in the range of 573-773 K, CuO, Cu 2O and ZnO crystallites were detected, and CuO and ZnO diffraction peak intensities and their crystalline sizes increased with the increase of calcination temperature, while Cu 2O crystalline might turn into CuO gradually. In the range of 573-873 K, calcination temperature had little influence on the specific surface area and pore volume of ultrafine CuO ZnO SiO 2 catalysts, but crystalline Zn 2SiO 4 appeared after calcination at 973 K, which caused remarkable decrease of the specific surface area and pore volume of catalysts and led to decrease of the activity of catalysts. Calcination temperature showed much greater influence on the activity of catalysts than on the product distribution of hydrgenation of carbon dioxide; the selectivity to methanol increased with the increase calcination temperature, while selectivity to CO decreased, and calcination at 773 K was favorable for methanol synthesis from hydrogenation of carbon dioxide over ultrafine CuO ZnO SiO 2 catalysts. TPR results as well as XRD patterns further confirmed the influences of calcination temperature on the interaction between CuO and ZnO, SiO 2, such as the formation of crystalline Zn 2SiO 4 and moreover on the reduction behaviour and activity of catalysts. Reduction temperature in the range of 548-648 K had little influence on the catalytic activity, but after reduction at 703 K Cu 0 might be formed and accounted for the decrease of catalytic activity.
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