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关于CePO催化剂上MOx(M = Mn、Co和Cu)改性用于NH3选择性催化还原NO的对比研究

A comparative study of MOx (M = Mn, Co and Cu) modifications over CePO catalysts for selective catalytic reduction of NO with NH.

作者信息

Liu Cheng, Li Fei, Wu Jing, Hou Xin, Huang Wei, Zhang Yong, Yang Xiangguang

机构信息

Northwest Research Institute of Chemical Industry, Xi'an, 710600, China.

Northwest Research Institute of Chemical Industry, Xi'an, 710600, China.

出版信息

J Hazard Mater. 2019 Feb 5;363:439-446. doi: 10.1016/j.jhazmat.2018.09.054. Epub 2018 Sep 24.

Abstract

The MO (M = Cu, Mn, Co)/CePO support was firstly prepared via the hydrothermal and impregnated method. Selective catalytic reduction of NO with NH (NH-SCR) results showed that the MnO modifications greatly improved the SCR activities at low temperatures. The NOx conversion of the MnO/CePO catalyst was above 80% even at 180 °C. In-situ DRIFTS results suggest that the SCR reaction is majorly conducted between the absorbed monodentate nitrate and NH species (i.e., the Langmuir-Hinshelwood mechanism). MOx (M = Cu, Mn, Co) exists in the formation of nano-size particles obtained by SEM and TEM directly. These nano-size particles can provide active surface adsorbed oxygen and thus improve the NO oxidation ability as indicated by the O-TPD and NO oxidation tests. The process of NO oxidation to NO plays a key role to produce the absorbed monodentate nitrate as indicated by the In-situ DRIFTS. The support CePO acts as the acid sites to form highly active NH species. The synergic effect between the MnO and CePO contributed to the high SCR activity over the MnO/CePO catalyst. Additionally, the MOx/CePO catalyst exhibits an excellent water tolerance and N selectivity. Consequently, the MnO/CePO catalyst becomes the potential catalyst for the practical process.

摘要

首先通过水热和浸渍法制备了MO(M = Cu、Mn、Co)/CePO载体。用NH₃选择性催化还原NO(NH₃-SCR)的结果表明,MnO改性极大地提高了低温下的SCR活性。即使在180℃时,MnO/CePO催化剂的NOₓ转化率仍高于80%。原位漫反射红外傅里叶变换光谱(DRIFTS)结果表明,SCR反应主要在吸附的单齿硝酸盐和NH₃物种之间进行(即朗缪尔-欣谢尔伍德机理)。通过扫描电子显微镜(SEM)和透射电子显微镜(TEM)直接观察发现,MOₓ(M = Cu、Mn、Co)以纳米尺寸颗粒的形式存在。这些纳米尺寸颗粒可提供活性表面吸附氧,因此如氧程序升温脱附(O-TPD)和NO氧化测试所示,可提高NO氧化能力。原位DRIFTS表明,NO氧化为NO₂的过程在产生吸附的单齿硝酸盐方面起着关键作用。载体CePO作为酸性位点形成高活性的NH₃物种。MnO和CePO之间的协同作用有助于MnO/CePO催化剂具有高SCR活性。此外,MOₓ/CePO催化剂表现出优异的耐水性和N₂选择性。因此,MnO/CePO催化剂成为实际工艺中的潜在催化剂。

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