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作 者:尹萌欣 刘东升[1] 赵东越 丁彤[1] 田野[1] 李新刚[1] YIN Mengxin;LIU Dongsheng;ZHAO Dongyue;DING Tong;TIAN Ye;LI Xingang(Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin Key Laboratory of Applied Catalysis Science & Technology,School of Chemical Engineering & Technology,Tianjin University,Tianjin 300072,China)
机构地区:[1]天津化工协同创新中心天津市应用催化科学与工程重点实验室天津大学化工学院
出 处:《高等学校化学学报》2019年第10期2170-2177,共8页Chemical Journal of Chinese Universities
基 金:国家自然科学基金(批准号:21878213)资助~~
摘 要:制备了一系列不同Cu掺杂量的Pt/Ba/CuxMg1-xAl2O4(x=0,0.1,0.3)催化剂,将其应用于高温NOx储存还原(NSR)反应,并探究了Cu掺杂量对催化剂NOx消除性能的影响.结果表明,储存组分Ba CO3在NSR过程中存在再分散现象.高温时催化剂的NOx消除性能取决于其NOx储存量,而不是NO氧化和NOx还原性能.高温时催化剂的NOx储存量与其上硝酸盐的热稳定性密切相关,Pt/Ba/Mg Al2O4上NOx主要以离子态硝酸盐形式存在,而掺杂Cu后催化剂上的NOx又增加了单齿硝酸盐的存在形式,单齿硝酸盐具有更高的热稳定性,因此掺Cu催化剂具有更大的NOx储存量.在450~500℃范围内,Cu的掺杂显著提高了Pt/Ba/Mg Al2O4的NOx消除性能;Pt/Ba/Cu0.1Mg0.9Al2O4催化剂的性能最佳,450℃时的NOx消除效率高达90%.A series of Pt/Ba/CuxMg1-xAl2O4 catalysts with Cu doping was synthesized and used in hightemperature NOx storage reduction reaction.The results demonstrate that Ba CO3,the NOxstorage component,redisperses in the NOx storage reduction process.Moreover,the De-NOx activity of the catalysts at high temperatures was determined by the NOx storage capacity,rather than the NO oxidation and NOx reduction ability of the catalysts.The NOx storage capacity of the catalysts is directly linked to the thermal stability of nitrate species stored on the catalysts.NOx mainly exists in the form of ionic nitrate species on Pt/Ba/Mg Al2O4,while NOx mainly co-exists as ionic nitrate and monodentate nitrate species on the Cu-doped catalysts.We discovered that monodentate nitrate species show higher thermal stability than ionic nitrate species.As a result,the Cu-doped catalysts exhibit the larger NOxstorage capacity and hence the higher De-NOx activity.At the temperature range from 450℃to 500℃,the addition of Cu greatly enhanced the NOxremoval percentage of the catalysts.Among all the catalysts,Pt/Ba/Cu0.1Mg0.9Al2O4 has the highest De-NOx activity with NOx removal percentage about 90%at 450℃.
关 键 词:高温 Cu掺杂量 Pt/Ba/CuxMg1-xAl2O4 热稳定性 NOx储存还原
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