MoOx状态调控及其对VOx/MoOx-TiO2催化剂脱硝性能和热稳定性的影响OACSTPCD
The Regulation of MoOx State and Its Effect on the Denitration Performance and Thermal Stability of VOx/MoOx-TiO2 Catalysts
将七钼酸铵分别用水和草酸溶液溶解后与TiO2复合制备MoOx-TiO2载体,通过浸渍法负载钒获得VOx/MoOx-TiO2催化剂;采用XRD、SEM、BET、XPS、H2-TPR和NH3-TPD表征手段研究催化剂的结构和性质,并考察了其脱硝活性和高温老化性能.结果表明,草酸助溶七钼酸铵制得的VMoTiO-F在210~510℃的脱硝效率大于80.0%,优于用水溶解制备的VMoTiH-F;VMoTiO-F表面存在较多的MoOx,可增强与VOx的相互作用,促进催化剂表面产生更多的低价态VOx和表面化学吸附氧(Oα)活性物种;VMoTiO-F中的VOx和MoOx相互作用还能提高低温氧化还原性能,有利于催化过程中的电子传递;VMoTiH-F相比VMoTiO-F有更多的MoOx进入TiO2晶格,提高TiO2的热稳定性,而VMoTiO-A中的锐钛矿TiO2在高温老化中被严重烧结甚至部分转变为惰性金红石晶型,导致表面酸性位损失和氧化还原性能降低,因此VMoTiH-A催化剂的脱硝性能明显优于VMoTiO-A.
Ammonium heptamolybdate was dissolved in water or oxalic acid solution,and then compounded with TiO2 to prepare MoOx-TiO2 support,and the VOx/MoOx-TiO2 catalysts were obtained after loading vanadium by impregnation method.The structure and properties of the catalysts were characterized by XRD,SEM,BET,XPS,H2-TPR and NH3-TPD,and its denitration activity and high temperature aging performance were investigated.The results showed that the denitrification efficiency of VMoTiO-F prepared by oxalic acid-assisted dissolution of(NH4)6Mo7O24 was greater than 80.0%at 210~510 ℃,which was better than that of VMoTiH-F prepared by water dissolution.Because there was more MoOx on the surface of VMoTiO-F,the interaction with VOx was enhanced,which promoted the production of more low-valence VOx and surface chemisorbed oxygen(Oα)active species on the surface of the catalyst.At the same time,the interaction between VOx and MoOx could also improve the low-temperature redox performance and facilitate the electron transfer in the catalytic process.After high temperature aging,VMoTiH-F had more MoOx into the TiO2 lattice than VMoTiO-F,which was helpful to improve the thermal stability of TiO2.However,anatase TiO2 in VMoTiO-A was seriously sintered or even partially transformed into inert rutile crystal during high temperature aging,resulting in the loss of surface acid sites and the reduction of redox properties.Therefore,the denitrification performance of VMoTiH-A catalyst was significantly higher than that of VMoTiO-A.
方萍;陈康欣;林雨婷;范楷浩;单承宇;刘雪松
绍兴文理学院 化学化工学院/先进催化材料与功能分子合成平台,浙江 绍兴 312000
化学工程
VOx/MoOx-TiO2氨选择性催化还原MoOx-TiO2复合载体活性VOx热稳定性
VOx/MoOx-TiO2NH3-SCRMoOx-TiO2 composite supportActive component VOxThermal stability
《石油化工高等学校学报》 2024 (004)
40-48 / 9
国家自然科学基金面上项目(52370115);浙江省教育厅科研项目(Y202043125);绍兴文理学院横向项目(010/2024横).
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