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铁负载对 Fe/ZSM-5 催化剂用于 NH3 选择性催化还原 NO 性能和结构的影响。

Effect of iron loading on the performance and structure of Fe/ZSM-5 catalyst for the selective catalytic reduction of NO with NH.

机构信息

Department of Energy and Power Engineering, Henan University of Science and Technology, Luoyang, 471003, China.

National Engineering Lab of Coal-fired Pollution Emission Reduction, Shandong University, Jinan, 250061, China.

出版信息

Environ Sci Pollut Res Int. 2019 Jan;26(2):1706-1715. doi: 10.1007/s11356-018-3513-x. Epub 2018 Nov 17.

Abstract

A series of Fe/ZSM-5 catalysts with different Fe contents were prepared by impregnation method. The catalysts were characterized by TEM, XRD, H temperature-programed reduction (H-TPR), temperature-programed desorption of ammonia (NH-TPD), and in situ diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS), and the catalytic activity test was also carried out on selective catalytic reduction (SCR) denitration device. Results showed that the single metal iron-supported ZSM-5 catalyst has high deNO activity in the medium-high temperature range, and the optimal loading of Fe active component is 10 wt%; the deNO efficiency over 80% at the range of 350-450 °C and 431 °C reaches the maximum of 96.91%. Iron species can be finely dispersed on the surface of the carrier as amorphous oxides, and the crystalline structure of zeolite is retained. The significant redox performance, highly dispersed nanoparticles, and rich Lewis acid sites on the surface of catalyst are favorable for the SCR denitration reaction. Fe/ZSM-5 10 wt% catalyst has rich Lewis acid sites and less B acid sites and Lewis acidic sites play an important role during the reaction. Only Eley-Rideal (E-R) mechanism existed during the NH-SCR reaction process, and there is no denitration reaction being accomplished by L-H mechanism at 150 °C.

摘要

采用浸渍法制备了一系列不同铁含量的 Fe/ZSM-5 催化剂。采用 TEM、XRD、H 程序升温还原(H-TPR)、氨程序升温脱附(NH-TPD)和原位漫反射红外傅里叶变换光谱(DRIFTS)对催化剂进行了表征,并在选择性催化还原(SCR)脱硝装置上进行了催化活性测试。结果表明,负载单一金属铁的 ZSM-5 催化剂在中高温范围内具有较高的脱氮活性,Fe 活性组分的最佳负载量为 10wt%;在 350-450°C 范围内,脱氮效率超过 80%,431°C 时达到最大值 96.91%。铁物种可以以无定形氧化物的形式精细分散在载体表面,沸石的晶体结构得以保留。催化剂表面具有显著的氧化还原性能、高度分散的纳米颗粒和丰富的路易斯酸位,有利于 SCR 脱硝反应。Fe/ZSM-5 10wt%催化剂具有丰富的路易斯酸位和较少的 B 酸位,路易斯酸性位在反应中起着重要作用。在 NH-SCR 反应过程中只存在 Eley-Rideal(E-R)机制,在 150°C 时没有通过 L-H 机制进行脱硝反应。

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