Promotion mechanism of CeO2 addition on the low temperature SCR reaction over MnOx/TiO2: a new insight from the kinetic study

被引:22
|
作者
Xiong, Shangchao [1 ]
Liao, Yong [1 ]
Dang, Hao [1 ]
Qi, Feihong [1 ]
Yang, Shijian [1 ]
机构
[1] Nanjing Univ Sci & Technol, Sch Environm & Biol Engn, Nanjing 210094, Jiangsu, Peoples R China
来源
RSC ADVANCES | 2015年 / 5卷 / 35期
关键词
SELECTIVE CATALYTIC-REDUCTION; NO REDUCTION; MN-CE/TIO2; CATALYST; OXIDE CATALYSTS; NITRIC-OXIDE; NH3; MNOX-CEO2; MN; PERFORMANCE; AMMONIA;
D O I
10.1039/c5ra01767j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
CeO2 addition showed a notable improvement on the low temperature selective catalytic reduction (SCR) performance of MnOx/TiO2. In this work, a new insight into the promotion mechanism was established from the steady state kinetic study. The kinetic rate constants of the SCR reaction through the Eley-Rideal mechanism, those of the SCR reaction through the Langmuir-Hinshelwood mechanism, and those of the non-selective catalytic reduction (NSCR) reaction over MnOx/TiO2 and MnOx-CeO2/TiO2 were obtained according to the steady state kinetic analysis. After comparing the reaction kinetic constants of NO reduction over MnOx/TiO2 and MnOx-CeO2/TiO2, the mechanism of the addition of CeO2 for NO reduction over MnOx/TiO2 was discovered according to the relationship between the reaction rate constants and the catalyst properties. Because the oxidation ability of MnOx/TiO2 increased, the rate constant of the SCR reaction over MnOx/TiO2 increased remarkably after CeO2 addition, resulting in a notable promotion of N-2 formation. The oxidation of NH3 to NH over MnOx/TiO2 required two Mn4+ cations on the adjacent sites. However, the probability of two Mn4+ cations occurring on the adjacent sites on MnOx/TiO2 obviously decreased after CeO2 addition, although the oxidation ability of MnOx/TiO2 increased. Therefore, the rate of N2O formation during NO reduction over MnOx/TiO2 did not vary notably after CeO2 addition. As a result, both the SCR activity and N-2 selectivity of NO reduction over MnOx/TiO2 improved after CeO2 addition.
引用
收藏
页码:27785 / 27793
页数:9
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