锰锆复合氧化物CO催化还原NO性能研究  

Performance of manganese-zirconium composite oxide in the catalytic reduction of NO by CO

作　　者：谈冠希 迟姚玲[1] 李双 易玉峰[1] 靳广洲[1] TAN Guan-xi;CHI Yao-ling;LI Shuang;YI Yu-feng;JIN Guang-zhou(School of Chemical Engineering,Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology,Beijing Institute of PetrochemicalTechnology,Beijing 102617,China)

机构地区：[1]北京石油化工学院化学工程系燃料清洁化及高效催化减排技术北京市重点实验室

出　　处：《燃料化学学报》2019年第10期1258-1264,共7页Journal of Fuel Chemistry and Technology

基　　金：国家重点基础研究发展计划(973计划，2012CB215002)资助~~

摘　　要：采用柠檬酸络合法制备了锰锆复合氧化物催化剂,用XRD、H2-TPR、XPS和SEM等技术进行了表征,研究了其CO催化还原NO性能。结果表明,MnOx主要以Mn3O4物相存在,Zr占比的增加会促进Mn3O4物相的分散,引起Mn3O4平均晶粒粒径减小;Mn主要有Mn2+、Mn3+、Mn4+离子价态形式,添加Cu和Ce后,(Mn3++Mn4+)含量和表面吸附氧(OA)含量增加,H2-TPR还原峰温度向低温区偏移,有利于催化活性的提升。Mn-Zr-O复合氧化物的CO催化还原NO活性较低,加入Cu后的Mn-Cu-Zr-O复合氧化物其CO催化还原NO的活性得到改善,而添加Ce后所制备的Mn-Cu-Ce-Zr-O复合氧化物的催化活性进一步提高;在350℃下、反应空速为18000h-1时,Mn-Cu-Ce-Zr-O复合氧化物表现出较好的CO催化还原NO活性,CO转化率达到了89.17%,NO转化率达到了91.70%。A series of manganese-zirconium composite oxides were prepared by citric acid complexing method and characterized by XRD,H2-TPR,XPS and SEM;their performance in the catalytic reduction of NO by CO was investigated.The results show that Mn 3O 4 is the main phase for MnO x in the Mn-Zr composite oxide;an increase in the Zr content can promote the dispersion of Mn 3O 4 and reduce the average grain size of Mn 3O 4.Mn may exist in the form of Mn2+,Mn 3+ and Mn 4+ ions;the content of (Mn 3++ Mn 4+) and the quantity of surface adsorbed oxygen (OA) increase after the addition of Cu and Ce,which is beneficial to enhancing the catalytic activity.The pristine Mn-Zr-O composite shows a relatively low activity in the catalytic reduction of NO by CO;after adding Cu,the Mn- Cu-Zr-O composite exhibits much higher activity than Mn-Zr-O;moreover,the activity of Mn-Cu-Ce-Zr-O composite is even enhanced by adding Ce.For the catalytic reduction of NO by CO over the Mn-Cu-Ce-Zr-O composite at 350 ℃ and with a space velocity of18000 h -1,the CO conversion and NO conversion are 89.17% and 91.70%,respectively.

关 键 词：锰锆复合氧化物 CO NO 催化还原 活性 

分 类 号：O643.36[理学—物理化学]