Inverse hysteresis during the NO oxidation on Pt under lean conditions

被引:85
作者
Hauptmann, W. [1 ,2 ]
Votsmeier, M. [1 ]
Gieshoff, J. [1 ]
Drochner, A. [2 ]
Vogel, H. [2 ]
机构
[1] Umicore AG & Co KG, D-63403 Hanau, Germany
[2] Tech Univ Darmstadt, Ernst Berl Inst Tech & Makromol Chem, D-64287 Darmstadt, Germany
关键词
NO oxidation; Deactivation; Diesel exhaust; Platinum; Monolithic catalyst; Inverse hysteresis; Micro-kinetic model; CATALYTIC-OXIDATION; NO+O-2 REACTIONS; PT(111) SURFACE; HIGH COVERAGES; ATOMIC OXYGEN; PT/AL2O3; PLATINUM; PT/BAO/AL2O3; O-2; DISPERSION;
D O I
10.1016/j.apcatb.2009.09.008
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
It is shown that a platinum catalyst operated under a transient temperature profile exhibits a hysteresis behavior. The catalytic activity during heat-up phases exceeds the activity of the cool down phases. This effect is the opposite of the well-known hysteresis that can be caused by the existence of multiple steady states or the thermal inertia of the catalyst. It is therefore referred to as 'inverse hysteresis'. If the catalyst is operated at one temperature for a longer time, a steady state activity is observed that is in-between the higher activity of the transient heat-up and the lower activity of the transient cool down. The most likely explanation for the observed hysteresis behavior is a reversible oxidation of the platinum surface by NO2 and a reduction of the platinum surface by NO. A micro-kinetic surface mechanism including the reversible surface oxidation has been developed and implemented in a monolith reactor model. The observed hysteresis effects can be quantitatively reproduced by the numerical model. If the feed contains CO/NO/O-2 an inverse hysteresis is observed for NO and CO oxidation. This means that in the presence of NO the hysteresis behavior of the CO oxidation switches from the typical standard hysteresis to an inverse hysteresis. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:22 / 29
页数:8
相关论文
共 39 条
[1]  
[Anonymous], TASCHENBUCH VERSUCHS
[2]   Experimental and kinetic study of NO oxidation on model Pt catalysts [J].
Bhatia, Divesh ;
McCabe, Robert W. ;
Harold, Michael P. ;
Balakotaiah, Vemuri .
JOURNAL OF CATALYSIS, 2009, 266 (01) :106-119
[3]  
Bourges P, 1998, STUD SURF SCI CATAL, V116, P213
[4]   A MOLECULAR-BEAM STUDY OF THE ADSORPTION AND DESORPTION OF OXYGEN FROM A PT(111)SURFACE [J].
CAMPBELL, CT ;
ERTL, G ;
KUIPERS, H ;
SEGNER, J .
SURFACE SCIENCE, 1981, 107 (01) :220-236
[5]  
CHATTERJEE D, 2001, THESIS RUBRECHT KARL
[6]  
Cooper B. J., 1989, 890404 SAE
[7]   Promotional effect of Sn on NO oxidation over Pt/Al2O3 as promising gas exhaust catalytic converter.: Selective Pt and Sn dispersion determination [J].
Corro, G ;
Elizalde, MP ;
Velasco, A .
REACTION KINETICS AND CATALYSIS LETTERS, 2002, 76 (01) :117-122
[8]   Mean field modeling of NO oxidation over Pt/Al2O3 catalyst under oxygen-rich conditions [J].
Crocoll, M ;
Kureti, S ;
Weisweiler, W .
JOURNAL OF CATALYSIS, 2005, 229 (02) :480-489
[9]  
CROCOLL M, 2003, THESIS U KARLSRUHE
[10]   The effect of metal oxide additives (WO3, MoO3, V2O5, Ga2O3)on the oxidation of NO and SO2 over Pt/Al2O3 and Pt/BaO/Al2O3 catalysts [J].
Dawody, J ;
Skoglundh, M ;
Fridell, E .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2004, 209 (1-2) :215-225