Reaction mechanism of NO decomposition over alkali metal-doped cobalt oxide catalysts

被引:64
|
作者
Haneda, M [1 ]
Kintaichi, Y [1 ]
Hamada, H [1 ]
机构
[1] Natl Inst AIST, Res Inst Innovat Sustainable Chem, Tsukuba, Ibaraki 3058565, Japan
关键词
direct decomposition; nitrogen monoxide; alkali metals; Co3O4; isotopic transient kinetic analysis;
D O I
10.1016/j.apcatb.2004.08.003
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 kinetics of NO decomposition were investigated over alkali metal-doped Co3O4 catalysts. For all the alkali metal-doped Co3O4 catalysts tested, the presence of 02 caused a decrease in the N-2 formation rate with reaction orders between -0.26 and -0.40. The reaction orders with respect to NO were between 1.21 and 1.47, which are higher than unity, suggesting that NO decomposition proceeds via a bimolecular reaction. The observation by in situ Fourier transform infrared (FT-IR) spectroscopy confirmed the presence of nitrite (NO2-) species on the surface under NO decomposition conditions. Isotopic transient kinetic analysis performed using (NO)-N-14 and (NO)-N-15 revealed that a surface-adsorbed species, probably NO2-, serves as an intermediate during NO decomposition. We proposed a reaction mechanism in which the reaction is initiated by NO adsorption onto alkali metals to form NO2- species, which migrates to the interface between the alkali metals and Co3O4, the active sites, and then react with the adsorbed NO species to form N-2. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:169 / 175
页数:7
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