Effect of aging on the NOx storage and regeneration characteristics of fully formulated lean NOx trap catalysts

被引:30
|
作者
Ji, Yaying [1 ]
Easterling, Vencon [1 ]
Graham, Uschi [1 ]
Fisk, Courtney [1 ]
Crocker, Mark [1 ]
Choi, Jae-Soon [2 ]
机构
[1] Univ Kentucky, Ctr Appl Energy Res, Lexington, KY 40511 USA
[2] Oak Ridge Natl Lab, Fuels Engines & Emiss Res Ctr, Knoxville, TN 37932 USA
关键词
Lean NOx trap; NOx storage; NOx reduction; Catalyst aging; Precious metal sintering; SPATIAL-DISTRIBUTION; THERMAL-STABILITY; SUPPORTED RHODIUM; PRECIOUS-METAL; PARTICLE-SIZE; REDUCTION; SULFUR; H-2; TEMPERATURE; CERIA;
D O I
10.1016/j.apcatb.2011.02.005
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
In order to elucidate the effect of washcoat composition on lean NO trap (LNT) aging characteristics. fully formulated monolithic LNT catalysts containing varying amounts of Pt, Rh and BaO were subjected to accelerated aging on a bench reactor. Subsequent catalyst evaluation revealed that in all cases aging resulted in deterioration of the NOx conversion as a consequence of impaired NOx storage and NOx reduction functions, while increased selectivity to NH3 was observed in the temperature range 250-450 degrees C. Elemental analysis, H-2 chemisorption and TEM data revealed two main changes which account for the degradation in LNT performance. First, residual sulfur in the catalysts, associated with the Ba phase, decreased catalyst NOx storage capacity. Second. sintering of the precious metals in the washcoat occurred, resulting in decreased contact between the Pt and Ba, and hence in less efficient NOx spillover from Pt to Ba during NOx adsorption, as well as decreased rates of reductant spillover from Pt to Ba and reverse NOx spillover during catalyst regeneration. For the aged catalysts, halving the Pt loading from 100 to 50 g/ft(3) was found to result in a significant decrease in overall NOx conversion, while for catalysts with the same 100 g/ft(3) Pt loading, increasing the relative amount of Pt on the NOx storage components (BaO and La-stabilized CeO2), as opposed to an Al2O3 support material (where it was co-located with Rh), was found to be beneficial. The effect of Rh loading on aged catalyst performance was found to be marginal within the range studied (10-20 g/ft(3)), as was the effect of BaO loading in the range 30-45 g/L. (c) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:413 / 427
页数:15
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