Influence of different supports on the physicochemical properties and denitration performance of the supported Mn-based catalysts for NH3-SCR at low temperature

被引:140
作者
Yao, Xiaojiang [1 ,2 ]
Kong, Tingting [1 ]
Yu, Shuohan [3 ]
Li, Lulu [3 ]
Yang, Fumo [1 ,2 ,4 ]
Dong, Lin [3 ]
机构
[1] Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Res Ctr Atmospher Environm, Fangzheng Ave 266, Chongqing 400714, Peoples R China
[2] Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
[3] Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210093, Jiangsu, Peoples R China
[4] Yangtze Normal Univ, Chongqing 408100, Peoples R China
基金
中国国家自然科学基金;
关键词
Mn-based catalysts; Different supports; Coordination status; Denitration performance; Low-temperature NH3-SCR; METAL-OXIDE CATALYSTS; MIXED-OXIDE; CARBON NANOTUBES; NO REDUCTION; SURFACE INTERACTION; MNOX-CEO2; CATALYST; EFFICIENT CATALYST; RATIONAL DESIGN; NH3; SCR;
D O I
10.1016/j.apsusc.2017.01.081
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The commonly used supports of SiO2, gamma-Al2O3, TiO2, and CeO2 were synthesized, and used for preparing MnOx/SiO2, MnOx/gamma-Al2O3, MnOx/TiO2, and MnOx/CeO2 catalysts with the purpose of investigating the influence of crystal structure and coordination status on the physicochemical properties and denitration performance of these supported Mn-based catalysts for low-temperature NH3-SCR. The obtained samples were characterized by XRD, Raman, BET, H-2-TPR, NH3-TPD, in situ DRIFTS, NO + O-2-TPD, XPS, and NH3-SCR model reaction. XRD results indicate that MnOx species can be highly dispersed on the surface of),gamma-Al2O3, TiO2, and CeO2, which is because that there are some octahedral and tetrahedral vacancy sites, octahedral vacancy site, and cubic vacancy site exist on the surface of defective spinel structure gamma-Al2O3, anatase TiO2, and cubic fluorite-type structure CeO2, respectively. However, there is no any vacancy site on the surface of SiO2 due to its unique SiO4 tetrahedral structure, which results in the appearance of crystalline beta-MnO2 on the surface of MnOx/SiO2 catalyst. Furthermore, H-2-TPR results exhibit obvious different reduction behavior among these supported Mn-based catalysts, which is explained by the coordination status of Mn species. Finally, NH3-SCR model reaction results show that MnOx/gamma-Al2O3 catalyst presents the best catalytic performance among these supported Mn-based catalysts due to its high dispersion, suitable reduction behavior, largest amount of acid sites, optimal NOx adsorption capacity, and abundant Mn4+ content.(C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:208 / 217
页数:10
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