Effect of CuMn2O4 spinel in Cu-Mn oxide catalysts on selective catalytic reduction of NOx with NH3 at low temperature

被引:92
作者
Fang, De [1 ,2 ]
Xie, Junlin [1 ,3 ]
Mei, Di [1 ,2 ]
Zhang, Yongming [1 ,2 ]
He, Feng [1 ,2 ]
Liu, Xiaoqing [3 ]
Li, Yumei [3 ]
机构
[1] Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Peoples R China
[2] Wuhan Univ Technol, Sch Mat Sci & Engn, Wuhan 430070, Peoples R China
[3] Wuhan Univ Technol, Res & Test Ctr Mat, Wuhan 430070, Peoples R China
关键词
SUPPORTED MANGANESE OXIDE; CARBON NANOTUBES; MNOX/TIO2; CATALYSTS; TRANSITION-METALS; MIXED OXIDES; SCR; MECHANISM; TIO2; OXIDATION; VANADIA;
D O I
10.1039/c4ra02824d
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Using the impregnation method, a series of Cu-Mn oxide catalysts were prepared and investigated for the selective catalytic reduction (SCR) of NOx with NH3 at temperatures ranging from 353 K to 453 K. The 0.05Cu-MnOx/TiO2 catalyst shows the highest activity and yields nearly 100% NOx conversion at 453 K using GHSV 40 000 h(-1), while the 0.20Cu-MnOx/TiO2 catalyst exhibits a certain level of potassium tolerance. In addition, the catalysts show favorable stability and water resistance. According to the XRD, EDS and SCR performance results, the existence of a new crystallized CuMn2O4 spinel phase is the dominant parameter for outstanding SCR activity between 413 K and 453 K. TPR, XPS and in situ DRIFT experiments indicate that CuMn2O4 is responsible for low reduction temperature, strong interaction between manganese oxides and copper oxides, high Mn3+ content and numerous acid sites on the surface. Compared with MnOx/TiO2 catalysts, Cu-Mn oxide catalysts could reduce the poisoning effect of potassium, illustrating that the CuMn2O4 phase may play a significant role in K-tolerance. Meanwhile, based on a certain level of potassium tolerance in CuMn2O4, an oxidation mechanism for NO is proposed due to the increase in Mn3+ and the special structure of a spinel oxide.
引用
收藏
页码:25540 / 25551
页数:12
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