铁铈复合氧化物催化剂SCR脱硝的改性研究

Study on the modification of iron-cerium mixed oxide catalyst for selective catalytic reduction of NO

  • 摘要: 利用共沉淀法制备了铁铈催化剂,考察添加钛、锆、钨和钼对其SCR脱硝的改性规律。结果表明,钨和钼的添加提高了铁铈催化剂高温脱硝性能,却使其低温活性有所降低;钛的添加对铁铈催化剂脱硝性能具有促进作用,尤其提高了其低温活性,并拓宽了其完全转化温度窗口,为最佳改性物。当钛的物质的量比逐渐由0.10增至0.40,铁铈钛催化剂低温脱硝效率先增大后减小,但其高温脱硝效率逐渐增大至100%,钛的最佳物质的量比为0.15。XRD和N2吸附分析结果表明,钛能优化铁铈催化剂的孔隙结构,增大其比表面积和比孔容,细化其孔径,并与催化剂中铁、铈氧化物形成良好的固溶体,从而提高了铁铈催化剂的SCR脱硝性能。Fe0.8Ce0.05Ti0.15Oz催化剂在150~400℃取得了高于90%的NOx转化率。

     

    Abstract: A series of iron-cerium mixed oxide catalysts modified titanium, zirconium, tungsten and molybdenum were prepared by co-precipitation. The selective catalytic reduction of NOx with NH3(NH3-SCR) activity of the catalysts were carried out in a fixed-bed quartz tube reactor. The research results indicated that the addition of tungsten and molybdenum could increase the high-temperature NH3-SCR activity of the iron-cerium mixed oxide catalysts, but decreased its low-temperature NH3-SCR activity. Titanium could improve the NH3-SCR activity of the iron-cerium mixed oxide catalyst within the range of reaction temperature, especially at low-temperature. Titanium was the most suitable assistant. When increasing the molar fraction of titanium from 0.10 to 0.40, the low-temperature NH3-SCR activity of iron-cerium-titanium mixed oxide catalysts firstly increased and then decreased while the high-temperature activity gradually increased to 100%, and the optimum molar fraction of titanium was 0.15. The results of X-ray diffraction(XRD) and N2 adsorption isotherms showed that the addition of titanium could optimize the pore structure of iron-cerium mixed oxide catalyst, and increased the BET surface and the pore volume of the iron-cerium mixed oxide catalyst, meanwhile refined its pore size. At the some cases, titanium could react with iron oxide and cerium oxide within the iron-cerium mixed oxide catalyst to form the solid solution. Therefore, the addition of titanium could enhance the NH3-SCR activity of iron-cerium mixed oxide catalyst. Under the condition of the test, more than 90% of NOx conversion could be achieved over Fe0.8Ce0.05Ti0.15Oz catalyst at the temperature range of 150~400℃.

     

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