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[利用原位漫反射红外傅里叶变换光谱研究NO在Cu-ZSM-5上的表面吸附和选择性催化反应]

[The surface adsorption and selective catalytic reaction of NO on Cu-ZSM-5 using in situ DRIFTS].

作者信息

Zhang Ping, Wang Le-Fu, Chen Yong-Heng

机构信息

Department of Environmental Science, Guangzhou University, Guangzhou 510006, China.

出版信息

Guang Pu Xue Yu Guang Pu Fen Xi. 2007 Jun;27(6):1102-5.

Abstract

The prepared Cu-ZSM-5 catalyst presents higher activity at low temperature during the selective catalytic reduction (SCR) of NO, and the conversion from NO to N2 is 70.6% at 613 K. The in situ diffuse reflectance FTIR spectroscopy (in situ DRIFTS) is an important method for studying surface adsorption of catalyst and mechanism of catalytic reaction, and was used to study the surface adsorbed species and the selective catalytic reduction reaction of NO on Cu-ZSM-5 catalyst in the presence of propene as reductant, with excess O2 and at 298-773 K. Based on the in-situ DRIFTS, a reaction mechanism is proposed that on Cu-ZSM-5, NO is first transformed to a series of NO(x) surface adsorbates, then these species react with the activating species of propene (C(x)H(y) or C(x)H(y)O(x)) to form organo-intermediates, including a process from organo-NH to organo-CN again to organo-NO(x) (organo-nitro or organo-nitrito), and finally these key intermediates react to form nitrogen. The role of Cu is to promote NO(x) content. Propene is easily activated on Cu-ZSM-5 with oxygen, and furthermore, the presence of oxygen is necessary to form organo-NO(x) intermediates.

摘要

制备的Cu-ZSM-5催化剂在低温下对NO的选择性催化还原(SCR)表现出更高的活性,在613K时NO向N2的转化率为70.6%。原位漫反射傅里叶变换红外光谱(原位DRIFTS)是研究催化剂表面吸附和催化反应机理的重要方法,用于研究在丙烯作为还原剂、过量O2存在且温度为298 - 773K条件下,Cu-ZSM-5催化剂上的表面吸附物种和NO的选择性催化还原反应。基于原位DRIFTS,提出了一种反应机理:在Cu-ZSM-5上,NO首先转化为一系列NO(x)表面吸附物,然后这些物种与丙烯的活化物种(C(x)H(y)或C(x)H(y)O(x))反应形成有机中间体,包括从有机-NH到有机-CN再到有机-NO(x)(有机硝基或有机亚硝酸酯)的过程,最后这些关键中间体反应生成氮气。Cu的作用是促进NO(x)的含量。丙烯在Cu-ZSM-5上容易被氧气活化,此外,氧气的存在对于形成有机-NO(x)中间体是必要的。

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