A mechanistic study on the simultaneous elimination of soot and nitric oxide from engine exhaust


The non-catalytic interaction between soot and nitric oxide (NO) resulting in their simultaneous elimination was studied on different types of reactive site present on soot. The reaction mechanism proposed previously was extended by including seven new reaction pathways for which the reaction energetics and kinetics were studied using density functional theory and transition state theory. This has led to the calculation of a new rate for the removal of carbon monoxide (CO) from soot. The new pathways have been added to our polycyclic aromatic hydrocarbon (PAH) growthmodel and used to simulate the NO–soot interaction to form CO, N2 and N2O. The simulation results show satisfactory agreement with experiment for the new CO removal rate. The NO–soot reaction was found to depend strongly on the soot site type and temperature. For a set of temperatures, computed PAH structures were analysed to determine the functional groups responsible for the decrease in the reactivity of soot with NO with increasing reaction time. In isothermal conditions, it was found that as temperature is increased, the number of oxygen atoms remaining on the soot surface decreases, while the number of nitrogen atoms increases for a given reaction time.

Keywords: aromatic site, DFT, kinetic Monte-Carlo, modelling, PAH, simulation, soot, NOx

Associated Projects: Quantum Chemistry, Engines, and Nanoparticles

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