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鋯摻雜鈦負載錳氧化物用于低溫選擇性催化還原NO

Manganese oxides supported on zirconium-doped titania for low ternperature selective catalytic reduction of NO

  • 摘要: 采用凝膠溶膠法制備TiO2以及摩爾比分別為1:1和4:1的TiO2-ZrO2三種載體,然后浸漬負載一定量的活性組分MnOx制備相應催化劑.通過X射線衍射和掃描電鏡對載體和催化劑進行表征,并進行氨氣低溫選擇性催化還原NO(NH3-SCR)實驗來考察催化劑的活性.三種載體中TiO2-ZrO2(4:1)的顆粒粒徑最小且高度分散,加入氧化鋯后,Zr4+離子取代Ti4+離子摻雜進入TiO2晶格內,引起TiO2晶格畸變,抑制TiO2晶型轉變,并促進載體上活性組分Mn的均勻分布,從而提高催化劑的低溫選擇性催化還原活性.TiO2-ZrO2(4:1)加入質量分數10%的Mn后催化劑的活性最高,在130℃采用該催化劑催化時NO的轉化率達到92.6%;150℃時通入體積分數10%的水蒸氣會降低10%Mn/TiO2-ZrO2(4:1)催化劑的活性,撤消后活性可逐漸恢復;而200℃時10%Mn/TiO2-ZrO2(4:1)的活性基本不受水蒸氣的影響.

     

    Abstract: Three kinds of carriers TiO2, TiO2-ZrO2 with the molar ratio of 1:1, and TiO2-ZrO2 with the molar ratio of 4:1 were prepared by a sol-gel method, and then the corresponding catalysts were obtained through loading a certain amount of active ingredient MnOx on the carriers. The carriers and catalysts were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). Some experiments on the selective catalytic reduction of NO with ammonia (NH3-SCR) were performed in order to investigate the activity of the catalysts. It is found that TiO2-ZrO2 (4:1) has the minimum particle size and its particles are highly dispersive among the three carriers. When adding ZrO2, Zr4+ ions dope into the TiO2 lattice by substituting Ti4+ ions, and thus the lattice distortion is triggered and the crystal transformation is restrained in the TiO2. Furthermore, Zr also promotes the dispersion of the active ingredient on the carrier, thereby improves the activity of the catalysts. The 10%Mn/TiO2-ZrO2(4:l) catalyst that adding 10% Mn to TiO2-ZrO2(4:l) has the highest activity among the three catalysts. The conversion of NO can reach 92.6% when catalyzed by this catalyst at 130℃. The activity of 10%Mn/TiO2-ZrO2(4:l) decreases when adding 10% of water vapor at 150℃, and it can restore when cutting off water vapor. But water vapor has no effect on the activity of 10%Mn/TiO2-ZrO2(4:l) at 200℃.

     

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