以SiO2为载体,利用共浸渍法制备了不同Cu、Ce摩尔比和含量的CuxCe1-xO2-x/SiO2(x=0~1)催化剂,在消除内、外扩散的条件下,评价了催化剂的CO催化氧化活性,求取了反应的活化能,并对催化剂的结构进行了表征.结果表明,CuxCe1-xO2-x/SiO2催化剂的活性和反应活化能与Cu、Ce摩尔比和CuxCe1-xO2-x含量都有关系,其中Cu、Ce摩尔比为1:1的25% Cu0.5Ce0.5O1.5/SiO2催化剂具有最好的催化活性和最低的反应活化能,CO能够在169℃时完全转化,反应的活化能为56.1kJ/mol.对于Cu0.5Ce0.5O1.5系列催化剂,活性组分含量较低时,催化剂的物相主要是CuO—CeO2固溶体,含量大于35%时开始有CuO物相生成.对于不同Cu、Ce摩尔比的催化剂,Cu摩尔含量较高时主要是CuO物相,Cu摩尔含量较低时主要是CuO—CeO2固溶体和CeO2物相.活性组分Ce和Cu之间、活性组分和载体之间存在着一定的相互作用,其对催化剂的活性和反应活化能有一定的影响.
A series of CuxCe1-xO2-x/SiO2(x = 0 -1) catalysts with different Cu/Ce molar ratios and CuxCe1-xO2-x ( x = 0 - 1 ) contents were prepared by co-impregnation method. The activity of obtained catalysts for the CO oxidation was evaluated and the activation energies of these catalysts were calculated by avoiding internal and external diffusions. The catalysts were characterized by X-ray diffraction (XRD) and temperature programmed reduction (TPR) methods. It was found that the catalytic activity and the activation energies were dependent not only on the Cu/Ce molar ratios, but also on the contents of CuxCe1-xO2-x (x = 0 -1 ). 25% Cu0.5Ce0.5O1.5/SiO2 catalyst with the lowest activation energy of 56. 1 kJ/mol exhibited the highest activity for catalytic oxidation of CO, and CO could be totally oxidized at 169 ℃. For the Cu0.5Ce0.5O1.5/SiO2 series catalysts, the main phase was CuO-CeO2 solid solution when the content of Cu0.5Ce0.5O1.5 was low, while the CuO phase started to appear when the Cu0.5 Ce0.5O1.5 content was higher than 35%. For the catalysts with different Cu/Ce molar ratios, CuO was the main phase when the content of Cu is high, while the main phases were CuO-CeO2 solid solution and CeO2 when the content of Cu is low. The interactions among Cu, Ce and the support had effects on the activity and the activation energies of the catalysts.