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Kinetic study of the nitric oxide oxidation between 288 and 323 K, under pressure, focus on the oxygen influence on the reaction rate constant
International Journal of Chemical Kinetics ( IF 1.5 ) Pub Date : 2020-02-24 , DOI: 10.1002/kin.21353
Esther Neyrolles 1 , José Lara Cruz 1 , Georgio Bassil 2 , François Contamine 1 , Pierre Cezac 1 , Philippe Arpentinier 3
Affiliation  

The sequestration of carbon dioxide fumes from oxyfuel combustion is used to reduce significantly the carbon dioxide emissions from coal‐fired power plants. Impurities like nitric oxide, present in the fumes, can cause technical difficulties during the capture, the treatment, the transport, and the storage steps of the CO2 fumes. The purpose of this study is to better understand the oxidation of nitric oxide under pressure in the presence of carbon dioxide and in the experimental condition of flue gas treatment. This reaction is known to be a third‐order reaction, two order in nitric oxide and first order in oxygen. To examine the effect of the temperature, the pressure and the volume fraction of oxygen on the rate constant of oxidation, k1, an autoclave is used. The first experiment studies the influence of the temperature between 288 and 323 K. The results found are in the form of an Arrhenius‐type equation: k1 = 810 exp(620/T) and are in agreement with the literature. Carbon dioxide does not seem to have an influence on the rate constant, whereas our experimental measurements indicate an influence of the volume fraction of oxygen. The rate constant decreases when the oxygen volume fraction increases by up to 10%. Then the rate constant remains constant. This observation allows us to conclude that the mechanism involving the mechanism with a dimer of NO as an intermediate is more likely to be the mechanism involved in the nitric oxide oxidation in our experimental conditions: high pressure and ambient temperature. The rate constant k2, k–2, and k3 were also estimated in these conditions.

中文翻译:

一氧化氮在288和323 K之间在压力下的动力学研究,着重于氧气对反应速率常数的影响

富氧燃烧产生的二氧化碳烟雾被隔离,可显着减少燃煤电厂的二氧化碳排放。烟雾中存在的一氧化氮之类的杂质可能会在CO 2烟雾的捕获,处理,运输和存储步骤中引起技术难题。这项研究的目的是为了更好地了解在存在二氧化碳的情况下,在烟气处理的实验条件下,一氧化氮的氧化。已知该反应是三阶反应,一氧化二氮为一级。为了检查温度,压力和氧气体积分数对氧化速率常数k 1的影响,使用高压灭菌器。第一个实验研究温度在288和323 K之间的影响。发现的结果采用Arrhenius型方程式:k 1  = 810 exp (620 / T并且与文献一致。二氧化碳似乎对速率常数没有影响,而我们的实验测量表明氧的体积分数有影响。当氧气体积分数增加最多10%时,速率常数会降低。然后速率常数保持恒定。该观察结果使我们可以得出结论,在我们的实验条件下(高压和环境温度),涉及以二聚体NO为中间体的机理更可能是一氧化氮氧化的机理。在这些条件下,还估计了速率常数k 2k –2k 3
更新日期:2020-02-24
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