低温等离子体协同Cu-Mn-Ce-Zr/TiO_2催化降解甲苯  

Catalytic degradation of toluene over Cu-Mn-Ce-Zr/TiO_2 coupled with low temperature plasma

作　　者：豆宝娟[1] 赵晨晨 张庆 闫宁娜 杨德宇 郝庆兰[1] DOU Bao-juan;ZHAO Chen-chen;ZHANG Qing;YAN Ning-na;YANG De-yu;HAO Qing-lan(Tianjin University of Science and Technology,Tianjin 300457,China)

机构地区：[1]天津科技大学,天津300457

出　　处：《燃料化学学报》2019年第5期598-604,共7页Journal of Fuel Chemistry and Technology

基　　金：中国博士后科学基金面上(2017M623284)资助~~

摘　　要：以TiO_2为载体,采用等体积浸渍法制备了负载型CuxMn_(1-x)Ce_(0.75)Zr_(0.25)/TiO_2(x=1.0、0.75、0.5、0.25、0)负载型催化剂,采用XRD、H_2-TPR、O_2-TPD和XPS等方法对催化剂进行了表征,并通过低温等离子体协同催化剂对大流量的甲苯模拟废气进行了催化降解反应研究。结果表明,Cu和Mn单主金属催化剂的活性优于Cu-Mn双主金属催化剂,其原因是双金属催化剂中Mn的添加减弱了Cu与助剂Ce之间的相互作用,使得催化剂的晶格氧减少,低温还原性能降低。在反应初期,甲苯降解主要依赖于催化剂的活性,具有较好的低温还原性以及丰富的氧空穴和晶格氧含量的CuCe_(0.75)Zr_(0.25)/TiO_2的活性最好; Mn具有较强的O_3分解能力,当等离子体比能密度(SED)增加到一定值后,等离子体与催化剂的协同作用增强,从而使得MnCe_(0.75)Zr_(0.25)/TiO_2催化剂活性高于CuCe_(0.75)Zr_(0.25)/TiO_2,强化了甲苯的脱除。A series of supported CuxMn1-xCe0.75Zr0.25/TiO2( x = 1. 0,0. 75,0. 5,0. 25,0) catalysts were prepared by impregnation and characterized by XRD,H2-TPR,O2-TPD and XPS;the performance of CuxMn1-xCe0.75Zr0.25/TiO2 catalysts in the degradation of toluene coupled with lowtemperature plasma under high space velocity was then investigated. The results indicate that the composite catalysts with single Cu or Mn as the main active component exhibit higher activity than those with double Cu and Mn components;the addition of second component may weaken the interaction between Cu and Ce,leading to a decrease in the content of lattice oxygen and the reducibility at lowtemperature. The CuCe0.75Zr0.25/TiO2 catalyst exhibits superior performance for toluene oxidation in the initial reaction stage,owing to its high content of lattice oxygen and oxygen vacancies. With the increase of the specific energy density( SED) of lowtemperature plasma,the concentration of O3 increases and the MnCe0.75Zr0.25/TiO2 catalyst then displays higher activity in toluene degradation than CuCe0.75Zr0.25/TiO2,because of the prominent enhancement of synergistic effect between plasma and catalyst over the former MnCe0.75Zr0.25/TiO2 catalyst.

关 键 词：低温等离子体 Cu-Mn双金属催化剂 协同催化 甲苯降解 

分 类 号：X511[环境科学与工程—环境工程]