Characterization and catalytic investigation of Fe-ZSM5 for urea-SCR

被引:134
作者
Devadas, Mukundan
Kroecher, Oliver [1 ]
Elsener, Martin
Wokaun, Alexander
Mitrikas, George
Soeger, Nicola
Pfeifer, Marcus
Demel, Yvonne
Mussmann, Lothar
机构
[1] Paul Scherrer Inst, CH-5232 Villigen, Switzerland
[2] Swiss Fed Inst Technol ETHZ Zurich, Phys Chem Lab, CH-8093 Zurich, Switzerland
[3] Umicore AG & Co KG, Automot Catalysts, D-63403 Hanau, Germany
关键词
Fe-ZSM5; ammonia; SCR; monolith; EPR; DRIFT; ammonia inhibition;
D O I
10.1016/j.cattod.2006.08.018
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Fe-ZSM5 was prepared with high iron content by solid-state ion exchange and characterized by ICP-AES, BET surface measurements, TEM, UV-vis. EPR and DRIFT spectroscopy as well as supplementing catalytic tests in order to clear up its functionality in urea-SCR. Due to the over-exchange with iron small Fe2O3 particles were formed, identified by UV-vis, EPR and TEM measurements, which were proved to be not active for the SCR reaction. However, the oxidation of NO to NO2 over Fe3+ ions in the catalyst was realized to be a pre-requisite for the SCR reaction and the rate-determining step. DRIFT investigations under SCR conditions showed adsorbates on Fe2+ up to 300 degrees C. The high SCR activity above 300 degrees C can be explained by the faster reoxidation of Fe2+ to Fe3+ sites at high temperatures. The observed inhibition of the SCR reaction by excess ammonia at low and intermediate temperatures can be explained in this context by the reducing properties of ammonia converting Fe3+ to Fe2+ or by preventing the reoxidation of Fe2+. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:137 / 144
页数:8
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