Elucidation of Lean-NOx reduction mechanism using kinetic isotope effect

被引:12
作者
Cho, BK [1 ]
机构
[1] GM Corp, Ctr Res & Dev, Phys & Phys Chem Dept, Warren, MI 48090 USA
关键词
D O I
10.1006/jcat.1998.2169
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 effect of an NO isotope on the kinetics of lean-NOx catalysis in (NO + C2H4 + O-2) reaction mixtures over Pt-ZSM-5 was theoretically analyzed and compared with experimental data obtained with a fixed-bed plug-flow reactor. The large kinetic isotope effect, as well as kinetic oscillations observed previously, was explained by NO decomposition kinetics on Pt surfaces which undergo phase transition between (1 x 1) and (hex) phases induced by adsorbed reactant species. Results indicate the importance of NO decomposition kinetics in lean-NOx catalysis, lending further support to a lean-NOx reduction mechanism which involves NO decomposition accompanied by hydrocarbon oxidation. (C) 1998 Academic Press.
引用
收藏
页码:395 / 407
页数:13
相关论文
共 44 条
[1]   MECHANISM OF THE LEAN NOX REACTION OVER CU/ZSM-5 [J].
ANSELL, GP ;
DIWELL, AF ;
GOLUNSKI, SE ;
HAYES, JW ;
RAJARAM, RR ;
TRUEX, TJ ;
WALKER, AP .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1993, 2 (01) :81-100
[2]   SELECTIVE REDUCTION OF NITROGEN-OXIDES UNDER OXIDIZING EXHAUST-GAS CONDITIONS [J].
BENNETT, CJ ;
BENNETT, PS ;
GOLUNSKI, SE ;
HAYES, JW ;
WALKER, AP .
APPLIED CATALYSIS A-GENERAL, 1992, 86 (02) :L1-L6
[3]   THE ROLE OF NO2 IN THE REDUCTION OF NO BY HYDROCARBON OVER CU-ZRO2 AND CU-ZSM-5 CATALYSTS [J].
BETHKE, KA ;
LI, C ;
KUNG, MC ;
YANG, B ;
KUNG, HH .
CATALYSIS LETTERS, 1995, 31 (2-3) :287-299
[4]   NO REDUCTION BY HYDROCARBONS IN AN OXIDIZING ATMOSPHERE OVER TRANSITION METAL-ZIRCONIUM MIXED OXIDES [J].
BETHKE, KA ;
ALT, D ;
KUNG, MC .
CATALYSIS LETTERS, 1994, 25 (1-2) :37-48
[5]   STRUCTURE SENSITIVITY OF NO ADSORPTION ON A SMOOTH AND STEPPED PT(100) SURFACE [J].
BONZEL, HP ;
BRODEN, G ;
PIRUG, G .
JOURNAL OF CATALYSIS, 1978, 53 (01) :96-105
[6]   SELECTIVE CATALYTIC REDUCTION OF NITRIC-OXIDE WITH ETHANE AND METHANE ON SOME METAL EXCHANGED ZSM-5 ZEOLITES [J].
BURCH, R ;
SCIRE, S .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 3 (04) :295-318
[7]   MECHANISM OF THE SELECTIVE REDUCTION OF NITROGEN MONOXIDE ON PLATINUM-BASED CATALYSTS IN THE PRESENCE OF EXCESS OXYGEN [J].
BURCH, R ;
MILLINGTON, PJ ;
WALKER, AP .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1994, 4 (01) :65-94
[8]   Activity normalization for lean-NOx catalysts [J].
Cho, BK .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 12 (2-3) :147-160
[9]   NITRIC-OXIDE REDUCTION BY ETHYLENE OVER CU-ZSM-5 UNDER LEAN CONDITIONS - STUDY OF REACTION DYNAMICS BY TRANSIENT EXPERIMENTS [J].
CHO, BK .
JOURNAL OF CATALYSIS, 1995, 155 (02) :184-195
[10]   Nitric oxide reduction by ethylene over Pt-ZSM-5 under lean conditions: Steady-state activity [J].
Cho, BK ;
Yie, JE .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1996, 10 (04) :263-280