Synergetic catalytic removal of chlorobenzene and NOx from waste incineration exhaust over MnNb0.4Ce0.2Ox catalysts: Performance and mechanism study

被引:31
作者
Yang, Bo [1 ]
Jin, Qijie [2 ,3 ]
Huang, Qiong [1 ]
Chen, Mindong [1 ]
Xu, Leilei [1 ]
Shen, Yuesong [2 ]
Xu, Haitao [2 ]
Zhu, Shemin [2 ]
Li, Xiujun [3 ]
机构
[1] Nanjing Univ Informat Sci & Technol, Jiangsu Collaborat Innovat Ctr Atmospher Environm, Sch Environm Sci & Engn, Jiangsu Key Lab Atmospher Environm Monitoring & P, Nanjing 210044, Peoples R China
[2] Nanjing Tech Univ, Coll Mat Sci & Engn, Jiangsu Collaborat Innovat Ctr Adv Inorgan Funct, Nanjing 210009, Peoples R China
[3] Univ Texas El Paso, Dept Chem & Biochem, Environm Sci & Engn & Biomed Engn, El Paso, TX 79968 USA
基金
中国国家自然科学基金;
关键词
Synergistic catalytic removal; Nitrogen oxides (NOx); Chlorobenzene (CB); Hydrothermal stability; Removal mechanism; Rare earths; LOW-TEMPERATURE SCR; CE-O-X; MIXED OXIDES; HYDROTHERMAL STABILITY; SUPPORTED MANGANESE; SO2; TOLERANCE; REDUCTION; NH3; OXIDATION; COMBUSTION;
D O I
10.1016/j.jre.2020.06.013
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Nb doped MnCe0.2Ox complex oxides catalysts prepared via a homogeneous precipitation method were investigated for synergistic catalytic removal of NOx and chlorobenzene (CB) at low temperatures. The MnNb0.4Ce0.2Ox catalyst with a molar ratio of Nb/Mn = 0.4 exhibits excellent activity and the NOx and CB removal efficiency reaches 94.5% and 96% at 220 degrees C, respectively. Furthermore, the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox still remains above 80% after injecting 300 ppm SO2 and 7 vol% H2O for 36 h. In addition, the presence of CB and NOx + NH3 can improve the NOx and CB removal efficiency of MnNb0.4Ce0.2Ox respectively. The analysis results from N-2-BET, Py-IR, H-2-TPR and NH3-TPD reveal that the introduction of Nb increases the average pore size, pore volume and surface area, promoted the growth of Lewis acid amount obviously, and enhances redox ability of MnCe0.2Ox at 100-250 degrees C. Moreover, the molecular migration process of NOx, NH3, CB and SO2 in NH3-SCR and CB oxidation reaction over MnNb0.4Ce0.2Ox catalysts were systematically studied. In situ DRIFTS, FT-IR and XPS also confirm that the adsorption of sulfate species and SO2 on the surface of MnNb0.4Ce0.2Ox is inhibited effectively by the introduction of Nb in the presence of SO2 and H2O. Moreover, Nb additives also enhance the structural stability of MnNb0.4Ce0.2Ox,( )due to the interactions among Mn, Nb and Ce. The NH3-TPD, H-2-TPR and in situ DRIFTS results also confirm that the MnNb0.4Ce0.2Ox still retains abundant acid sites and high redox ability in the presence of SO2 and H2O. In summary, MnNb0.4Ce0.2Ox catalysts represent a promising and effective candidate for controlling NOx and CB at low temperatures. (C) 2020 Chinese Society of Rare Earths. Published by Elsevier B.V. All rights reserved.
引用
收藏
页码:1178 / 1189
页数:12
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