不同类型含铁分子筛上N2O催化分解反应

doi:10.1016/S1872-2067(12)60555-5

催化学报 ›› 2013, Vol. 34 ›› Issue (5): 876-888.DOI: 10.1016/S1872-2067(12)60555-5

不同类型含铁分子筛上N₂O催化分解反应

王俊英^a,b, 夏海岸^a, 鞠晓花^a, 范峰滔^a, 冯兆池^a, 李灿^a

a 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023;
b 中国科学院大学, 北京 100049

收稿日期:2012-12-26 修回日期:2013-05-20 出版日期:2013-05-06 发布日期:2013-05-06
通讯作者: 李灿
基金资助:
国家自然科学基金(21173213);国家重点基础研究发展计划(973计划,2009CB623507).

Catalytic performance of different types of iron zeolites in N₂O decomposition

WANG Junying^a,b, XIA Haian^a, JU Xiaohua^a, FAN Fengtao^a, FENG Zhaochi^a, LI Can^a

a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
b Graduate University of Chinese Academy of Sciences, Beijing 100049, China

Received:2012-12-26 Revised:2013-05-20 Online:2013-05-06 Published:2013-05-06
Supported by:
This work was supported by the National Natural Science Foundation of China (21173213) and the National Basic Research Program of China (973 Program, 2009CB623507).

摘要/Abstract

摘要：

采用固态离子交换法制备了一系列Fe/Al摩尔比为0.33的Fe/分子筛(ZSM-35,ZSM-5,beta和mordenite (丝光沸石))样品,并利用紫外-可见漫反射光谱、原位红外光谱和可见拉曼光谱以及瞬态应答实验考察了分子筛种类对N₂O分解反应性能的影响.研究表明,经高温处理(HT)后分子筛的催化活性顺序为 Fe/ZSM-35 > Fe/beta > Fe/ZSM-5 > Fe/mordenite,与骨架外铝稳定的双核铁物种含量一致.这说明双核铁物种是高温处理后Fe/分子筛样品中N₂O分解的活性位,而它的形成与分子筛种类密切相关.Fe/ZSM-35分子筛十元环孔道中相邻两个α位和八元环孔道中相邻两个β位都能稳定两个Fe(II)离子而形成能高效分解N₂O的双核铁活性中心.Fe/beta和Fe/ZSM-5分子筛中只有落在相邻两个β位上的两个Fe(II)离子才能形成参与N₂O分解的高活性的双铁活性中心.Fe/mordenite-HT分子筛上的铁物种绝大部分以孤立Fe离子的形式存在,因此其催化N₂O分解反应活性很低.

关键词: 铁, 分子筛, 氧化亚氮分解, 拉曼光谱

Abstract:

A series of Fe/zeolites (ZSM-35, ZSM-5, beta, and mordenite) samples with Fe/Al molar ratios of 0.33 were prepared using a solid-state ion-exchange method. A combination of ultraviolet-visible diffuse reflectance, in-situ Fourier-transform infrared, and in-situ visible Raman spectroscopic techniques, with a transient response method, was used to investigate the influence of the zeolite framework on the catalytic properties of the Fe/zeolites in N₂O decomposition. The results show that the catalytic activity of the Fe/zeolites-HT (HT denotes high-temperature treatment) samples is in the order Fe/ZSM-35-HT > Fe/beta-HT > Fe/ZSM-5-HT > Fe/mordenite-HT. There is a linear relationship between the rate of N₂O decomposition and the concentration of binuclear iron sites. This indicates that binuclear iron sites are the active sites for N₂O decomposition. A correlation between the formation of binuclear iron sites and Fe ion distribution among the cationic sites is proposed. Two Fe(II) cations located in two adjacent six-membered rings in a 10-membered ring channel (α sites) or in two neighboring six-membered rings in an eight-membered ring channel (β sites) of Fe/ZSM-35 are favorable for the formation of active binuclear iron sites. Similar structure can also be formed in two adjacent six-membered rings in polymorphs A and B of beta zeolite or in the six-membered rings at the intersection of the straight and sinusoidal channels of the ZSM-5 framework. For the Fe/mordenite-HT sample, most of the iron species are present as isolated iron cations, so it has the lowest activity in N₂O decomposition.

Key words: Iron, Zeolite, Nitrous oxide decomposition, Raman spectroscopy

王俊英, 夏海岸, 鞠晓花, 范峰滔, 冯兆池, 李灿. 不同类型含铁分子筛上N₂O催化分解反应[J]. 催化学报, 2013, 34(5): 876-888.

WANG Junying, XIA Haian, JU Xiaohua, FAN Fengtao, FENG Zhaochi, LI Can. Catalytic performance of different types of iron zeolites in N₂O decomposition[J]. Chinese Journal of Catalysis, 2013, 34(5): 876-888.

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不同类型含铁分子筛上N₂O催化分解反应

Catalytic performance of different types of iron zeolites in N₂O decomposition

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