不同类型含铁分子筛上N2O催化分解反应
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...
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| Published in | 催化学报 Vol. 34; no. 5; pp. 876 - 888 |
|---|---|
| Main Author | |
| Format | Journal Article |
| Language | Chinese |
| Published |
中国科学院大学,北京100049%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
2013
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 |
| Subjects | |
| Online Access | Get full text |
| ISSN | 0253-9837 1872-2067 |
| DOI | 10.1016/S1872-2067(12)60555-5 |
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| Abstract | 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. |
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| AbstractList | 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. 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. |
| Author | 王俊英 夏海岸 鞠晓花 范峰滔 冯兆池 李灿 |
| AuthorAffiliation | 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 中国科学院大学 |
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| Author_FL | LI Can WANG Junying FENG Zhaochi JU Xiaohua XIA Haian FAN Fengtao |
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| DocumentTitleAlternate | Catalytic performance of different types of iron zeolites in N2O decomposition |
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| EISSN | 1872-2067 |
| EndPage | 888 |
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| Keywords | 氧化亚氮分解 铁 Iron Zeolite Nitrous oxide decomposition Raman spectroscopy 分子筛 拉曼光谱 |
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| Notes | 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 21-1195/O6 Iron Zeolite Nitrous oxide decomposition Raman spectroscopy 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 |
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| Publisher | 中国科学院大学,北京100049%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 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 |
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| SubjectTerms | 分子筛 拉曼光谱 氧化亚氮分解 铁 |
| Title | 不同类型含铁分子筛上N2O催化分解反应 |
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