Effect of extra-framework gallium on the structure of iron species in Fe/ZSM-5

Effect of extra-framework gallium on the structure of iron species in Fe/ZSM-5
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骨架外镓对 Fe/ZSM-5 中铁物种结构的影响

DOI:
10.1016/j.jcat.2008.09.001
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发表时间:
2008-10
影响因子:
7.3
通讯作者:
Su, Weiguang
Su, Weiguang
中科院分区:
化学1区
文献类型:
--
作者:
Sun, Keqiang;Fan, Fengtao;Sun, Keju;Ying, Pinliang;Li, Can;Feng, Zhaochi;Xia, Haian;Su, Weiguang

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采用固态离子交换法制备了一系列不同Ga含量的Fe/Ga- zsm -5催化剂。采用紫外和可见光拉曼光谱、紫外-可见光漫反射光谱、h2 -程序升温还原和523 K下N2O分解等方法研究了框架外Ga对Fe/Ga- zsm -5催化剂中Fe物种性质的影响。在Fe/Ga- zsm -5中引入超框架Ga和高温处理对Fe的分布甚至性质都有显著影响。对于高温处理的催化剂,外框架Ga的存在显著增加了Fe(II)位的数量和N2O直接分解活性,表明外框架Ga可以促进N2O分解活性位的形成。对框架外Ga的有益作用的可能解释是,框架外Ga促进了双核和寡核Fe(III)位点的还原,形成Fe(II)位点,并与低核Fe位点相互作用,形成高温处理催化剂的Fe - Ga - o混合相。
A series of Fe/Ga-ZSM-5 catalysts with different Ga contents were prepared by solid-state ion exchange method. Ultraviolet and visible Raman spectroscopy, ultraviolet–visible diffuse reflectance spectroscopy, H2-temperature-programmed reduction, and N2O decomposition at 523 K were used to investigate the effect of extra-framework Ga on the nature of the Fe species in Fe/Ga-ZSM-5 catalysts. Introducing extra-framework Ga and high-temperature treatment can significantly affect the distribution even the nature of the Fe species in Fe/Ga-ZSM-5. For the high-temperature treated catalysts, the presence of extra-framework Ga remarkably increases the amount of the Fe(II) sites and the activity of direct N2O decomposition, suggesting that extra-framework Ga can promote the formation of the active sites for N2O decomposition. The possible interpretation of the beneficial role of extra-framework Ga is that extra-framework Ga facilitates the reduction of bi- and oligo-nuclear Fe(III) sites to form the Fe(II) sites and interacts with the Fe sites with low nuclearity to form a mixed Fe–Ga–O phase for the high-temperature treated catalysts.
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