A mechanistic study on the simultaneous elimination of soot and nitric oxide from engine exhaust
A mechanistic study on the simultaneous elimination of soot and nitric oxide from engine exhaust
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DOI：
10.1016/j.carbon.2010.12.005
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发表时间：
2011-04
期刊：
影响因子：
10.9
通讯作者：
A. Raj;Z. Zainuddin;Markus Sander;M. Kraft
中科院分区：
文献类型：
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作者：
A. Raj;Z. Zainuddin;Markus Sander;M. Kraft
研究了烟灰与一氧化氮（NO）的非催化相互作用，并对烟灰上不同类型的活性位点进行了研究。对先前提出的反应机理进行了扩展，增加了7种新的反应途径，并利用密度泛函理论和过渡态理论研究了反应的能量学和动力学。这导致了从煤烟中去除一氧化碳（CO）的新速率的计算。这些新途径被添加到我们的多环芳烃（PAH）生长模型中，并用于模拟NO-soot相互作用形成CO， n2和N2O。模拟结果与实验结果吻合较好。无灰反应与灰点类型和温度有很大关系。对于一组温度，分析了计算的多环芳烃结构，以确定随着反应时间的增加，烟灰与NO的反应性降低的官能团。在等温条件下，发现在一定的反应时间内，随着温度的升高，烟灰表面保留的氧原子数量减少，而氮原子数量增加。
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, N2and 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.