Formation of reactive Lewis acid sites on Fe/WO3-ZrO2 catalysts for higher temperature SCR applications

被引:68
作者
Foo, Rodney [1 ]
Vazhnova, Tanya [1 ]
Lukyanov, Dmitry B. [1 ]
Millington, Paul [2 ]
Collier, Jillian [2 ]
Rajaram, Raj [2 ]
Golunski, Stan [3 ]
机构
[1] Univ Bath, Dept Chem Engn, Catalysis & React Engn Grp, Bath BA2 7AY, Avon, England
[2] Johnson Matthey Technol Ctr, Reading RG4 9NH, Berks, England
[3] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales
关键词
Selective catalytic reduction; Nitrogen oxide; Iron; Tungsten zirconia; Acidity; PROMOTED SULFATED ZIRCONIA; N-PENTANE ISOMERIZATION; TUNGSTEN-OXIDE; NITRIC-OXIDE; BUTANE ISOMERIZATION; FE-ZSM-5; CATALYSTS; NH3-SCR REACTION; SURFACE-ACIDITY; BETA CATALYST; REDUCTION;
D O I
10.1016/j.apcatb.2014.06.034
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
Tungsten-zirconia (WO3-ZrO2), which oxidises NH3 but shows no NOx-reduction activity, can be converted into an active ammonia-SCR catalyst by impregnation with Fe. The role of Fe in inducing SCR activity has been studied by relating the catalytic performance of tungsten-zirconia materials (containing 0, 0.5, 2,3 and 10 wt% Fe) to their surface acidity, which has been probed by pyridine adsorption. The most active material, 3 wt% Fe/WO3-ZrO2, reduces NOx by 10-20% at the minimum temperature tested (150 degrees C), and achieves 80-85% conversion at temperatures between 400 and 550 degrees C. The performance can be correlated with the formation of new Fe3+ Lewis acid sites that have a pivotal role in the SCR reaction by activating NOx, and which are associated with a characteristic peak shift in the IR spectrum of adsorbed pyridine. The introduction of Fe also has the effect of increasing the strength of the Bronsted acidity, which accounts for the similarity in activity observed between the Fe/WO3-ZrO2 materials and benchmark Fe/beta-zeolite catalysts at higher temperatures. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:174 / 179
页数:6
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