A kinetic study of NO formation during oxy-fuel combustion of pyridine

A kinetic study of NO formation during oxy-fuel combustion of pyridine
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吡啶富氧燃烧过程中NO生成的动力学研究

DOI:
10.1016/j.apenergy.2011.11.039
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发表时间:
2012-04
期刊:
影响因子:
11.2
通讯作者:
Fei, H.
Fei, H.
中科院分区:
工程技术1区
文献类型:
--
作者:
Wang, B.;Sun, L. S.;Su, S.;Xiang, J.;Hu, S.;Fei, H.

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采用流动反应器,在1073- 1473 K温度范围内,以O2/CO2为反应气氛,研究了吡啶-N转化为NO和N2的反应动力学,并对不同化学计量比下的NO生成途径进行了分析。实验结果表明,较高的温度促进了NO的生成,富燃和贫燃条件下NO的转化率分别为1.26-18.64%和3.85-43%。对于N2的生成,在氧化气氛下,从1073到1173 K,吡啶转化为N2的转化率略有增加,然后迅速下降,而在氧气不足的情况下,该转化率稳定在36%左右,然后在1173 K以上下降到29%。在O2/Ar和O2/CO2气氛中,随着当量比的增加,NO浓度单调增加,且两种气氛间的差距随α的增大而增大。模拟结果表明,高CO2浓度通过促进HNO+M参与H+NO+M反应和限制HNO+O2参与HO 2 + NO反应,降低了氧气的利用率,从而改变了NO的生成,这在较高温度下更为重要.此外,NO消耗的主要途径是通过与NCO和NH作为中间体的反应。总的来说,Terasa 09的模型很好地描述了实验趋势,并且该燃烧动力学适用于富氧燃料条件。
In this work, pyridine-N was converted into NO and N2by using a flow reactor and the dominant NO evolution pathways were identified by means of a kinetic modeling under O2/CO2atmosphere in temperature range of 1073–1473K for different stoichiometries. The experimental results indicated higher temperatures promoted the formation of NO, with conversions varied from 1.26–18.64% to 3.85–43% for fuel-rich and fuel-lean conditions respectively. As for N2formation, conversion of pyridine to N2had a slight increase from 1073 to 1173K then declined rapidly in oxidizing atmosphere, whereas this conversion stabilized at about 36% before decreasing to 29% above 1173K in the presence of insufficient O2. Increasing the equivalence ratio led to a monotonic increase of NO in both O2/Ar and O2/CO2atmospheres, and the gap between these atmospheres developed with α. The simulation results showed that the high CO2concentration reduced the availability of oxygen thus altered the evolution of NO through promoting reaction HNO+M↔H+NO+M and limiting reaction HNO+O2↔HO2+NO. This was even more important at higher temperatures. Besides, the major pathways for NO consumption were taken through reaction with NCO and NH as intermediates. In general, the model of Terasa09 described the experimental trends well, and this combustion kinetic was applicable to oxy-fuel conditions.
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