PNNL

Abstract

Modern technologies use NO2 to promote low temperature soot oxidation for diesel particulate filter regeneration. Most previous methods studied soot oxidation with NO2 using offline methods such as thermo-gravimetric analysis (TGA). In this study, the online aerosol-technique of high-temperature oxidation tandem differential mobility analysis (HTO-TDMA) is used to study kinetics of soot oxidation with NO2 under N2 environment. This method has significant advantages over previous offline methods in reducing heat and mass transfer diffusion limitations to the soot surface. Soot particles are exposed to varying temperature and NO2 concentration inside the furnace resulting from thermal decomposition of NO2 to NO. This causes soot oxidation rates to vary throughout the furnace. In this study, variations in temperatures, NO2 concentrations and particle residence times are thoroughly accounted for the first time, and soot oxidation rates are derived. Soot oxidation rate is calculated as a function of Arrhenius rate constant Asoot, activation energy Esoot, and partial pressure of NO2 PNO2 within the furnace at temperatures ranging 500- 950 C. Results suggest Asoot and Esoot values for soot oxidation with NO2 of 1.68 nm K-0.5 s-1 (Nm-2)-n and 46.5 kJ mol-1 respectively. The activation energy for soot oxidation with NO2 is significantly lower than oxidation with air. However, ppm levels of NO2 cause soot oxidation at low temperatures suggesting NO2 is a stronger oxidant than O2. This study also shows that a semi-empirical approach with just a few kinetic parameters could represent varying soot oxidation rates in a diesel engine cylinder or on a diesel particulate filter. Further studies should be directed towards understanding synergistic effects of other oxidants as O2 and H2O in addition to NO2 using the HTO-TDMA method.