Insight into the SO2 resistance mechanism on γ-Fe2O3 catalyst in NH3-SCR reaction: A collaborated experimental and DFT study

被引:145
作者
Yu, Yaxin [1 ]
Tan, Wei [1 ]
An, Dongqi [1 ]
Wang, Xiuwen [1 ]
Liu, Annai [1 ]
Zou, Weixin [1 ,3 ]
Tang, Changjin [1 ,3 ]
Ge, Chengyan [4 ]
Tong, Qing [2 ]
Sun, Jingfang [1 ,2 ]
Dong, Lin [1 ,2 ,3 ]
机构
[1] Nanjing Univ, Lab Mesoscop Chem, MOE, Sch Chem & Chem Engn, Nanjing 210093, Peoples R China
[2] Nanjing Univ, Ctr Modern Anal, Jiangsu Key Lab Vehicle Emiss Control, Nanjing 210093, Peoples R China
[3] Nanjing Univ, Sch Environm, Nanjing 210093, Peoples R China
[4] Yancheng Inst Technol, Sch Chem & Chem Engn, Yancheng 224051, Peoples R China
基金
中国国家自然科学基金;
关键词
gamma-Fe2O3; SO2; resistance; Competitive adsorption; Surface acidity; Dynamic equilibrium; AMMONIUM BISULFATE FORMATION; LOW-TEMPERATURE NH3-SCR; V2O5-MOO3/TIO2; CATALYST; REDUCTION; NOX; NH3; SCR; DECOMPOSITION; CO; TOLERANCE;
D O I
10.1016/j.apcatb.2020.119544
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
SO2 poisoning of NH3-SCR catalysts at low temperature (< 300 degrees C) is still an austere challenge. In this work, gamma-Fe2O3 was taken as a model catalyst and the effect of reaction temperature on the catalytic activity in the presence of SO2 were fully revealed. SO2 introduction has no negative effect on the activity at 300 degrees C, which gradually improves with the extension of time. While for 225-275 degrees C, the activity decreases firstly and then increases slowly. The formatted sulfate species inhibits the adsorption of NOx, cuts off L-H reaction pathway and leads to the initial decline. While the deposited ammonium bisulfate (ABS) can be consumed continuously by NO + O-2, implying the formation and consumption of ABS have reached a dynamic equilibrium. Moreover, the formation of ferric sulfate species results in the enhancement of surface acidity, which leads to the promotion of the E-R reaction pathway and further facilitates the increase of activity.
引用
收藏
页数:11
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