Selective catalytic oxidation (SCO) of ammonia to nitrogen over Fe-exchanged zeolites prepared by sublimation of FeCl3
Selective catalytic oxidation (SCO) of ammonia to nitrogen over Fe-exchanged zeolites prepared by sublimation of FeCl3
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DOI：
10.1016/j.jcat.2004.05.023
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发表时间：
2004-08-15
影响因子：
7.3
通讯作者：
Yang, RT
中科院分区：
文献类型：
--
作者：
Qi, GS;Gatt, JE;Yang, RT
通过升华 FeCl3 制备铁交换沸石，并研究其在氧气存在下作为氨选择性催化氧化 (SCO) 生成氮气的催化剂。通过FeCl3在700℃升华制备的Fe-ZSM-5在非常高的空速(GHSV = 2.3 x 10(5) h(-1))下表现出优异的SCO性能。在400℃下获得了超过99%的NH3转化率和接近100%的N-2选择性。在不同温度(括号内，C)升华制备的Fe-ZSM-5催化剂中，催化性能按Fe-ZSM-5(700)>Fe-ZSM-5(600)>Fe-ZSM-5(500)、Fe-ZSM-5(400)、Fe-ZSM-5(350)的顺序降低。 700℃升华制备的不同Fe沸石催化剂中，催化性能依次降低为Fe-ZSM-5>Fe-MOR>Fe-FER>Fe-Beta>Fe-Y，与水性离子交换法制备的Fe沸石催化剂相似。还研究了不同铁沸石上 NO 与氨的 SCR（选择性催化还原）活性。 FTIR结果支持两步机制：NO是N-2形成的中间体，NH3首先被O-2氧化成NO，NO然后与未反应的NH3反应生成N-2。 (C) 2004 Elsevier Inc. 保留所有权利。
Fe-exchanged zeolites were prepared by subliming FeCl3 and studied as catalysts for selective catalytic oxidation (SCO) of ammonia to nitrogen in the presence of oxygen. Fe-ZSM-5 prepared by sublimation of FeCl3 at 700 degreesC showed excellent SCO performances at a very high space velocity (GHSV = 2.3 x 10(5) h(-1)). Over 99% NH3 conversion and nearly 100% N-2 selectivity were obtained at 400 degreesC. Among Fe-ZSM-5 catalysts prepared by subliming at different temperatures (denoted in parentheses, in C), the catalytic performance decreased in the sequence of Fe-ZSM-5 (700) > Fe-ZSM-5 (600) > Fe-ZSM-5 (500), Fe-ZSM-5 (400), Fe-ZSM-5 (350). Among different Fe-zeolite catalysts prepared by subliming at 700 C, the catalytic performance decreased in the sequence of Fe-ZSM-5 > Fe-MOR > Fe-FER > Fe-Beta > Fe-Y which are similar to the Fe-zeolites prepared by aqueous ion-exchange method. The activity for the SCR (selective catalytic reduction) of NO with ammonia was also investigated on different Fe-zeolites. The FTIR results supported the two-step mechanism: NO is an intermediate for N-2 formation, NH3 was first oxidized to NO by O-2, NO then reacts to the unreacted NH3 to produce N-2. (C) 2004 Elsevier Inc. All rights reserved.