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CuY和Cu-ZSM-5催化剂上NO直接分解活性及活性中心的研究
THE CATALYTIC ACTIVITY FOR NO DECOMPOSITION AND ACTIVE SITES OVER CuY AND CuZSM-5
【摘要】 研究了CuY,Cu-ZSM-5分子筛制备条件对NO直接分解活性的影响.结果表明,在不同酸碱度下交换的CuY分子筛,在pH=9时活性较好,而Cu-ZSM-5型在pH=7时较好.随交换度提高,Cu-ZSM-5活性上升,而CuY交换度达45%后活性趋于平稳:用DTA,TPD,XPS及IR等技术,对活性中心进行了研究,表明钢是以水合离子形式与分子筛中Na+进行交换.Cu-ZSM-5的活性位单一,CuY上则有两种NO吸附位.经400℃焙烧后,铜优先占据Y的β笼,此即活性位.未经焙烧的样品中铜主要以Cu2+存在.400℃抽空处理产生Cu+.讨论了NO在含铜样品表面的反应过程.
【Abstract】 he effect of catalyst preparation condition on the catalytic activity for NO direct decomposition over CuY, CuZSM-5 was studied by use of quadrupole MS as means of activity measurement in a recycling low pressure reaction system. It was showed that the activity of catalysts prepared at different PH is best at pH=9 for CuY and at pH=7 for CuZSM-5 respectively. With the increase of exchange level of copperon, the activity of CuZSM-5 and CuY increases, but the activity of CuY dose not increase any longer after the exchange level reaches 45%.The characteristic of active sites was studied by using DTA, TPD, XPS and IR techniques. It was supposed that the copper as hydrated ionexchanges with Na+ of zeolites; only one kind of copper ion site locates in CuZSM-5 and two kinds locate in CuY; the copper ions firstly occupy the 3 cage of Y zeolite and the activity is provided by the copper ions in 3 cage; copper exists as cupric ions in fresh sample and cuprous ions appear through pretreatment at hightemperature in vacuum. Five kinds of NO adsorbed species were detected by in-situ IR at 20-350℃. Amongthe species, the NO+/Cu2+ was one of the active species.
【Key words】 zeolite; CuY; CuZSM-5; nitrogen oxide; direct decomposition; active site;
- 【文献出处】 催化学报 ,CHINESE JOURNAL OF CATAL YSIS , 编辑部邮箱 ,1994年06期
- 【分类号】O643.36
- 【被引频次】29
- 【下载频次】233