In situ FT-IR investigation of the reduction of NO with CO over Au/CeO2-Al2O3 catalyst in the presence and absence of H2

被引:40
|
作者
Kantcheva, M. [1 ]
Samarskaya, O. [1 ]
Ilieva, L. [2 ]
Pantaleo, G. [3 ]
Venezia, A. M. [3 ]
Andreeva, D. [2 ]
机构
[1] Bilkent Univ, Dept Chem, TR-06800 Ankara, Turkey
[2] BAS, Inst Catalysis, Sofia 1113, Bulgaria
[3] CNR, Ist Studio Mat Nanostrutturati, I-90146 Palermo, Italy
关键词
Ceria; Ceria-alumina; Supported gold; NO reduction by CO; Mechanism; In situ FT-IR spectroscopy; GAS SHIFT REACTION; SUPPORTED GOLD CATALYSTS; NITRIC-OXIDE; CARBON-MONOXIDE; SPECTROSCOPIC CHARACTERIZATION; POLLUTION-ABATEMENT; SURFACE COMPLEXES; METAL-OXIDES; CERIA; ISOCYANATE;
D O I
10.1016/j.apcatb.2008.09.023
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
The NO + CO + H-2 reaction over CeO2, Au/CeO2 (3 wt% Au), Au/CeO2-Al2O3 (2.9 wt% Au, 20 wt% Al2O3) and CeO2-Al2O3 mixed support prepared by co-precipitation has been Studied by FT-IR spectroscopy at elevated temperatures. Formation of NCO species has been detected on all of the samples. The presence of metallic gold is not necessary for the generation of the isocyanates on ceria and the mixed ceria-alumina support. The NCO species are produced by a process involving the dissociation of NO on the oxygen vacancies of the support, followed by the reaction between N atoms lying oil the surface and CO molecules. Gold plays an important role in the modification of ceria leading to Ce3+ and oxygen vacancies formation, and causes significant lowering of the reduction temperature of CeO2 and CeO2-Al2O3 enhancing the reducibility of ceria surface layers. The role of H-2 is to keep the surface reduced during the course of the reaction. The onset temperature, at which the interaction between the surface isocyanates and No begins, is low (100 degrees C). This explains the high activity of the Au/CeO2-Al2O3 catalyst with 100% selectivity in the reduction of NO by CO at low temperature (200 degrees C) and in the presence of H-2 (C) 2008 Elsevier B.V. All rights reserved
引用
收藏
页码:113 / 126
页数:14
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