NOx adsorption on Pt/K/Al2O3

被引:60
|
作者
Toops, TJ [1 ]
Smith, DB [1 ]
Partridge, WP [1 ]
机构
[1] Oak Ridge Natl Lab, Fuels Engines & Emiss Res Ctr, Knoxville, TN 37932 USA
关键词
lean NOx traps; DRIFTS; chemisorption; potassium; NOx storage;
D O I
10.1016/j.cattod.2006.02.006
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
This study explores NO(x)storage in a Pt/K/Al2O3 lean NOx trap (LNT) catalyst using in situ diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS) in conjunction with chemisorption. The combination of these techniques allows the quantification of surface species for this catalyst system. A free nitrate ion, NO3-, is the primary form of stored No, on the potassium phase at all temperatures, but there was significant nitrite formation observed below 200 degrees C during short adsorption times. The NO2 saturation storage on Pt/K/Al2O3 decreases from 6.7 mu mol/m(2) at 150 degrees C to 1.8 mu mol/m(2) at 400 degrees C, and DRIFTS indicates that the equilibrated surface species are identical over this entire temperature range. While the final state of Pt/K/Al2O3 is identical at all temperatures, the rates and observed surface species change significantly. After 1 min uptake, NO, adsorption varies from 0.35 mu mol/m(2) at 150 degrees C to a maximum of 3.2 mu mol/m(2) at 250 degrees C, and at 400 degrees C the adsorption decreases to 1.1 mu mol/m(2). This temperature sweep illustrates the limiting regimes associated with NOx adsorption: kinetic limitations at lower temperatures due to the strength of the Pt-O bond and insufficient storage sites at higher temperatures. This study propose three routes for the storage of NOx on Pt/K/Al2O3, two of them involving a potassium storage site adjacent to Pt sites, and a third route that involves a form of NO2 disproportionation on storage sites irrespective of their proximity to Pt. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:112 / 124
页数:13
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