烧蚀型载体烟气脱硝催化剂的制备与性能研究
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摘要
本文制备并研究了NH3-SCR脱硝粉体催化剂和蜂窝体催化剂，分别考察了原位溶胶-凝胶法制备的V2O5/TiO2催化剂和分步浸渍法制备V2O5-WO3/TiO2催化剂的催化性能。针对分步浸渍催化剂制备过程，采用不同载体、不同活性组分前驱体及烧蚀型载体负载方式制备了相应的V2O5-WO3/TiO2催化剂，通过N2吸附、XRD、NH3-TPD、H2-TPR、紫外-可见光分析、SEM、In-situ FTIR等表征手段对以上粉体催化剂进行评价。结果显示：原位溶胶-凝胶制备的催化剂具有介孔结构、脱硝活性温度窗口宽，但原料成本高且WO3难以原位负载；不同载体分步浸渍法制备的催化剂中介孔TiO2制备的催化剂具有较宽的活性温度窗口与抗硫抗水中毒稳定性；烧蚀型载体负载制备的催化剂兼具原位溶胶-凝胶法与浸渍法制备催化剂的优点，且抗硫抗水性能稳定。对烧蚀型载体负载制备的粉末催化剂与廉价黏土通过掺混制备蜂窝体催化剂并进行考察，得出掺混70wt.%黏土A制得的蜂窝体催化剂性能较好，具有稳定的抗硫抗水中毒性能，建立了低成本高性能蜂窝体脱硝催化剂的制备工艺。同时，用烧蚀型载体负载制备的粉末催化剂涂覆在黏土蜂窝体表面制得了涂覆蜂窝催化剂，通过评价发现涂层厚度增加到110μm时涂覆催化剂与100%挤出成型蜂窝催化剂的活性相当。
Powder and honeycomb NH3-SCR catalysts were prepared in this paper, and both in-situsol-gel method and two-step impregnation method were adopted in the preparation of the powdercatalyst. The two-step impregnation method was optimized by varying the supports and theirstructures, the precursors of active component and the method utilizing combustible carrier. Allcatalysts were characterized with XRD, UV-Vis, in-situ FTIR, SEM, NH3-TPD and H2-TPR todeeply understand the structure, acidity, redox property and reaction mechanism involving inNH3-SCR of NO. The results show that the catalysts made by the in-situ sol-gel method hadmesoporous structure, high dispersion of V2O5on the surface of TiO2and wide window ofworking temperatures, but the method itself is expensive. The two-step impregnation method hasthe feature of low cost, and the prepared V2O5-WO3/TiO2catalyst on mesoporous TiO2allowedalso a wide working-temperature window. Using combustible carrier to facilitate the dispersion ofTiO2support further made the resulting catalyst have activity and performances of denitrationsimilar to that of the catalysts made by the sol-gel method. Then, honeycomb catalyst wasprepared by the extrusion method based on blending clay and the powder catalyst facilitated usinga combustible carrier. Testing the effect of different clays on the preparation process and thehoneycomb catalyst itself found that the catalyst blending70wt.%clay well met the requirementof industrial application for de-NOx of flue gas. A coating honeycomb catalyst was also tested,demonstrating that its activity increased with increasing the coating thickness and the catalyst witha thickness of110μm enabled the comparably good activity as the extruded honeycomb of100%powder catalyst. This indicates thus a possible low-cost technology for making honeycomb.
Powder and honeycomb NH3-SCR catalysts were prepared in this paper, and both in-situsol-gel method and two-step impregnation method were adopted in the preparation of the powdercatalyst. The two-step impregnation method was optimized by varying the supports and theirstructures, the precursors of active component and the method utilizing combustible carrier. Allcatalysts were characterized with XRD, UV-Vis, in-situ FTIR, SEM, NH3-TPD and H2-TPR todeeply understand the structure, acidity, redox property and reaction mechanism involving inNH3-SCR of NO. The results show that the catalysts made by the in-situ sol-gel method hadmesoporous structure, high dispersion of V2O5on the surface of TiO2and wide window ofworking temperatures, but the method itself is expensive. The two-step impregnation method hasthe feature of low cost, and the prepared V2O5-WO3/TiO2catalyst on mesoporous TiO2allowedalso a wide working-temperature window. Using combustible carrier to facilitate the dispersion ofTiO2support further made the resulting catalyst have activity and performances of denitrationsimilar to that of the catalysts made by the sol-gel method. Then, honeycomb catalyst wasprepared by the extrusion method based on blending clay and the powder catalyst facilitated usinga combustible carrier. Testing the effect of different clays on the preparation process and thehoneycomb catalyst itself found that the catalyst blending70wt.%clay well met the requirementof industrial application for de-NOx of flue gas. A coating honeycomb catalyst was also tested,demonstrating that its activity increased with increasing the coating thickness and the catalyst witha thickness of110μm enabled the comparably good activity as the extruded honeycomb of100%powder catalyst. This indicates thus a possible low-cost technology for making honeycomb.
引文
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