Mn-Ce/(CC-A)@12TiO_2整体式蜂窝催化剂的制备及脱硝性能研究  

Preparation and performance for NO_x removal of Mn-Ce/(CC-A)@12TiO_2 monolith honeycomb catalyst

作　　者：李星颖 牟文涛[1] 李凯 张申[1] 郭玉玉[1] 吴旭[1] 李哲[1] LI Xing-ying;MU Wen-tao;LI Kai;ZHANG Shen;GUO Yu-yu;WU Xu;LI Zhe(College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学化学化工学院,山西太原030024

出　　处：《应用化工》2018年第11期2329-2335,共7页Applied Chemical Industry

基　　金：国家自然科学国家重点项目(21336006);山西省科学技术攻关项目(20140313002-2);中国自然科学基金(21106174;21177136);中国科学院战略领导科技项目(XDA07030300)

摘　　要：以氨水预处理后的堇青石蜂窝陶瓷为基体,采用半原位溶胶-凝胶工艺制备涂覆TiO_2涂层的Mn-Ce/(CC-A)@12TiO2整装脱硝催化剂,在80～260℃,NOx转化率达90%以上。N2吸脱附、XRD、TG-DSC等分析测试表明,TiO_2主要以结构完整的锐钛矿晶型存在,促进了活泼氧物质的生成,提高了催化活性。SEM图像表明,催化剂表面TiO_2涂层上具有裂纹和粗糙表面,有利于三维结构以及更多孔结构的形成,为反应物与活性位之间相互作用产生更多的活性中间体,从而促进反应速率提供了适宜的场所。EDS研究显示,催化剂Mn-Ce/(CC-A)@12TiO2中TiO_2表面形成的弱结晶Mn-Ce混合氧化物可能有利于Mn与Ce的微观协同效应,提高中间体的形成。Pretreating of CC with NH3·H2O and coating of TiO2 with semi-in-situ sol-gel method over CC-A were propitious to low-temperture catalytic performance of NH 3-SCR over monolith catalyst Mn-Ce/(CC-A)@12TiO2,with above 90%conversion of NO x during 80~260℃.Results of N 2-adsorption/desorption,XRD and DSC indicated that TiO2 mainly existed in intact anatase crystalline which accelerated the generation of labile oxygen species with contribution to activity.SEM images demonstrated that three-dimensional structure and more channels were formed over catalyst surface due to fissures and rough surface of special TiO 2 coating,which was conducive to interaction between reactants and active sites generating more reactive intermediates to accelerate reaction rate.EDS result showed that,Mn-Ce mixed oxides with weak crystalline over Mn-Ce/(CC-A)@12TiO2 might facilitate the synergistic effect between Mn and Ce to enhance the formation of intermediates as well.

关 键 词：整体式蜂窝状催化剂 堇青石 半原位溶胶-凝胶法 低温NH3的选择性催化还原 TIO2涂层 Mn-Ce/(CC-A)@12TiO2 

分 类 号：TQ032.41[化学工程] TQ137.12