Simulation of lean NOx trap performance with microkinetic chemistry and without mass transfer.

Larson, Rich ; Daw, C. Stuart (Oak Ridge National Laboratory, Knoxville, TN) ; Pihl, Josh A. (Oak Ridge National Laboratory, Knoxville, TN) ; Chakravarthy, V. Kalyana (Oak Ridge National Laboratory, Knoxville, TN)

关键词: BARIUM OXIDES;    CERIUM OXIDES;    CHEMICAL REACTIONS;    CHEMISTRY;    KINETICS;    MASS TRANSFER;    OXYGEN;    PERFORMANCE;    REGENERATION;    SIMULATION;    STEADY FLOW;    STORAGE;    THERMODYNAMICS;    TRANSIENTS;   

DOI  :  10.2172/1029795
RP-ID  :  SAND2011-5575
PID  :  OSTI ID: 1029795
Others  :  TRN: US201201%%205

学科分类：化学（综合）

美国|英语

来源: SciTech Connect

【 摘 要 】

A microkinetic chemical reaction mechanism capable of describing both the storage and regeneration processes in a fully formulated lean NO{sub x} trap (LNT) is presented. The mechanism includes steps occurring on the precious metal, barium oxide (NO{sub x} storage), and cerium oxide (oxygen storage) sites of the catalyst. The complete reaction set is used in conjunction with a transient plug flow reactor code to simulate not only conventional storage/regeneration cycles with a CO/H{sub 2} reductant, but also steady flow temperature sweep experiments that were previously analyzed with just a precious metal mechanism and a steady state code. The results show that NO{sub x} storage is not negligible during some of the temperature ramps, necessitating a re-evaluation of the precious metal kinetic parameters. The parameters for the entire mechanism are inferred by finding the best overall fit to the complete set of experiments. Rigorous thermodynamic consistency is enforced for parallel reaction pathways and with respect to known data for all of the gas phase species involved. It is found that, with a few minor exceptions, all of the basic experimental observations can be reproduced with these purely kinetic simulations, i.e., without including mass-transfer limitations. In addition to accounting for normal cycling behavior, the final mechanism should provide a starting point for the description of further LNT phenomena such as desulfation and the role of alternative reductants.