摘要
采用3种不同的浸渍过程制备了系列WO3改性MnOx/TiO2催化剂,并采用BET比表面积测试、X射线衍射、拉曼光谱、H2程序升温还原、高分辨扫描电镜和原位红外光谱等技术进行表征.结果显示,一步浸渍法和先钨后锰的分布浸渍法制备的催化剂中,Mn和W的协同作用提高了活性组分的分散状态,并阻止了钛载体的转晶;在所有的Mn基催化剂中,Mn物种主要以Mn2O3形式存在,但在15%MnOx-5%WO3/TiO2中出现了少量的MnO2;WO3的加入大大增强了催化剂的还原能力,提高了其表面酸位尤其是B酸的数量与强度,并促进了活性中间物(NH2)的生成.表面Lewis酸在低温SCR反应起主要作用,并且发现NH2也是活性很高的物种.在NH3低温催化还原NO的反应中,一步浸渍法制备的催化剂活性最高.
A series of WO3-modified MnOx/TiO2 catalysts were prepared by three different impregnation methods and were investigated by specific surface area measurement, X-ray diffraction, laser Raman spectroscopy, H2 temperature-programmed reduction, high-resolution transmission electron microscopy, and in situ Fourier transform infrared spectroscopy. The three-component catalysts obtained with the one-step impregnation exhibited the best catalytic activity. The characterization data revealed that a synergism between tungsten and manga- nese oxide existed in the catalysts when tungsten was loaded either prior to or simultaneously with manganese, which made the active com- ponents better dispersed and blocked the transformation of TiO2 from the anatase to rutile structure. The manganese oxide existed in the form of Mn203 on all the samples but was accompanied by a small amount of MnO2 for 15%MnOx-5%WO3/TiO2. WO3 improved the reducibility and enhanced the amount and strength of the surface acid sites, especially the Broensted acid sites and promoted the formation of the active intermediate （-NH2）. Lewis acid sites had the major role in the low temperature selective catalytic reduction reaction while surface -NH2 was an important intermediate species.
出处
《催化学报》
SCIE
EI
CAS
CSCD
北大核心
2012年第9期1523-1531,共9页
基金
国家高技术研究发展计划(863计划,2007AA061802)
江苏省自然科学基金重点项目(BK2008001)~~
关键词
钨氧化物
改性
锰氧化物
低温选择性催化剂还原
表面酸位
活性中间产物
tungsten oxide
modification
manganese oxide
low-temperature selective catalytic reduction
surface acidity
active intermediate
