Impact of dopants on catalysts containing Ce1-xMxO2-3 (M = Fe, Sb or Bi) in NH3-SCR of NOx-A multiple spectroscopic approach

被引:11
作者
Keller, Sonja [1 ]
Bentrup, Ursula [1 ]
Rabeah, Jabor [1 ]
Brueckner, Angelika [1 ,2 ]
机构
[1] Leibniz Inst Katalyse EV, Albert Einstein Stra 29a, D-18059 Rostock, Germany
[2] Univ Rostock, Dept Life Light & Matter, Albert Einstein Str 25, D-18059 Rostock, Germany
关键词
Ceria solid solutions; Supported vanadia; Low-temperature NH 3-SCR; Raman; In situ DRIFTS; In situ EPR; Mechanism; Surface oxygen; LOW-TEMPERATURE NH3-SCR; OXYGEN STORAGE CAPACITY; CERIA-BASED CATALYSTS; VANADIUM-OXIDE; REACTION-MECHANISM; NITRIC-OXIDE; LOCAL-STRUCTURE; SOLID-SOLUTIONS; RAMAN-SPECTRA; MIXED OXIDES;
D O I
10.1016/j.jcat.2021.04.026
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
Ce1-xMxO2-3 solid solutions (M = Fe3+, Bi3+, Sb3+; x = 0.01, 0.03, 0.05) with and without VOy surface species were characterized by standard techniques and tested in low-temperature NH3-SCR of NOx. In situ DRIFTS and EPR measurements at elevated temperature in the presence of different feed components allowed to identify active sites and structure-reactivity relationships. Catalytic activity of V-free supports follows the order CeSb > CeFe > CeO2 > CeBi and correlates with the formation of Ce-O surface species which promote initial NO oxidation. VOy/Ce1-xMxO2-3 catalysts are more active than corresponding V-free supports, yet the order of NOx conversion (VSbCe > VCe > VFeCe > VBiCe) is governed by the efficiency of the V5+/V4+ redox shuttle which is faster in VOy/Ce1-xSbxO2-3 than in VOy/CeO2 but lower when M = Fe and Bi. Activity of V-free supports is raised by increasing Bronsted acidity after treatment with H2O/SO2 containing feed while no positive effect was observed for VOy/Ce1-xMxO2-3, since the redox properties of VOy dominate over the impact of surface acidity. (c) 2021 Elsevier Inc. All rights reserved.
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页码:453 / 464
页数:12
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