TY - JOUR
T1 - A mechanistic study on the simultaneous elimination of soot and nitric oxide from engine exhaust
AU - Raj, Abhijeet
AU - Zainuddin, Zakwan
AU - Sander, Markus
AU - Kraft, Markus
N1 - KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: A.R. is grateful to Cambridge Commonwealth Trusts (CCT) and Clare College, Cambridge for their financial support. The authors highly acknowledge the support of EPSRC under EP/C547241/1 and EP/E01724X/1.
PY - 2011/4
Y1 - 2011/4
N2 - 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) growth model 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. © 2010 Elsevier Ltd. All rights reserved.
AB - 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) growth model 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. © 2010 Elsevier Ltd. All rights reserved.
UR - http://hdl.handle.net/10754/561738
UR - https://linkinghub.elsevier.com/retrieve/pii/S0008622310008717
UR - http://www.scopus.com/inward/record.url?scp=79551688571&partnerID=8YFLogxK
U2 - 10.1016/j.carbon.2010.12.005
DO - 10.1016/j.carbon.2010.12.005
M3 - Article
SN - 0008-6223
VL - 49
SP - 1516
EP - 1531
JO - Carbon
JF - Carbon
IS - 5
ER -