The synthesis of CuyMnzAl1−zOx mixed oxide as a low-temperature NH3-SCR catalyst with enhanced catalytic performance

催化作用 选择性催化还原 化学 X射线光电子能谱 氮氧化物 氧化物 无机化学 吸附 傅里叶变换红外光谱 过渡金属 核化学 物理化学 化学工程 生物化学 有机化学 工程类 燃烧
作者
Qinghua Yan,Sining Chen,Lei Qiu,Yanshan Gao,Dermot O’Hare,Qiang Wang
出处
期刊:Dalton Transactions [Royal Society of Chemistry]
卷期号:47 (9): 2992-3004 被引量:62
标识
DOI:10.1039/c7dt02000g
摘要

A new type of low-temperature selective catalytic reduction (SCR) catalyst, CuyMnzAl1-zOx, derived from layered double hydroxides is presented in this contribution. By tuning the Cu/Mn/Al ratio, the optimal catalyst Cu2Mn0.5Al0.5Ox resulted in a NOx conversion of 91.2% at 150 °C, which is much higher than that of all other control catalysts, Cu2AlOx (71.1%), Cu-Mn/γ-Al2O3 (65.23%), and Mn/γ-Al2O3 (59.32%). All samples were characterized in detail using various physico-chemical techniques including XRD, BET, FTIR, TEM, H2-TPR, NH3-TPD, and XPS analyses, and the results revealed that the superior catalytic performance of the Cu2Mn0.5Al0.5Ox catalyst can be attributed to its high specific surface area, high reducibility of MnO2 and CuO species, abundance of surface acid sites, and the good dispersion of MnO2 and CuO species. FTIR analyses of pyridine adsorbed samples revealed that the catalytic activity is proportional to the amount of Lewis acid sites. Cu2Mn0.5Al0.5Ox also showed much higher resistance to 100 ppm SO2 and 5% H2O than the control catalysts. The poisoning mechanism and the regenerability of the Cu2Mn0.5Al0.5Ox catalyst was also investigated. In all, compared with the control catalysts of Cu2AlOx, Cu-Mn/γ-Al2O3, and Mn/γ-Al2O3, the newly designed Cu2Mn0.5Al0.5Ox catalyst is not only more active at low temperatures (100-250 °C), but is also relatively more robust in the presence of SO2 and H2O.

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