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The behavior and modelling of the vibrational-to-translational temperature ratio at long time scales in CO2 vibrational kinetics
Reaction Chemistry & Engineering ( IF 3.9 ) Pub Date : 2019-09-21 , DOI: 10.1039/c9re00255c
Sergio H. Moreno 1, 2, 3, 4, 5 , Andrzej I. Stankiewicz 1, 2, 3, 4, 5 , Georgios D. Stefanidis 6, 7, 8, 9
Affiliation  

Non-thermal microwave plasma reactors can efficiently split the CO2 molecule. However, big challenges remain before this technology can become a feasible industrial technology. Computer modelling can be very useful to tackle such challenges. Detailed kinetic modelling is commonly used to gain insights into the complex vibrational kinetics of CO2, as vibrational excitation is strongly related to the energy efficiency in the dissociation process. The vibrational-to-translational temperature ratio has been identified as a key variable to achieve high energy efficiencies. This ratio has also been used to simplify detailed CO2 vibrational kinetics, notably reducing the number of species and reactions required to model the non-thermal plasma. In this paper we use an isothermal reaction kinetics model to study the vibrational kinetics of CO2 under the typical conditions used in non-thermal microwave plasma experiments. The importance of the different collisional processes is evaluated with respect to the different conditions and timescales at which CO2 dissociation takes place. The long timescale behavior of the vibrational-to-translational temperature ratio under different conditions is discussed in detail. It is shown that the behavior at increasing gas temperatures can be fitted to an expression that incorporates the Landau–Teller temperature dependence. This is confirmed by the average adjusted R-square values higher than 0.99 and the average root mean square error values smaller than 0.22 at low gas temperatures. The limitations of the fitting expression are also discussed, especially the conditions and timescales at which it yields better results.

中文翻译:

CO2振动动力学中较长时间尺度上的振动-平移温度比的行为和建模

非热微波等离子体反应器可以有效地分解CO 2分子。然而,在该技术成为可行的工业技术之前,仍然存在着巨大的挑战。计算机建模对于解决此类挑战非常有用。通常使用详细的动力学建模来深入了解CO 2的复杂振动动力学,因为振动激发与解离过程中的能量效率密切相关。振动和平移温度比已被确定为实现高能效的关键变量。该比率也已用于简化详细的CO 2振动动力学,显着减少了建模非热等离子体所需的物种数量和反应。在本文中,我们使用等温反应动力学模型来研究在非热微波等离子体实验中使用的典型条件下,CO 2的振动动力学。针对发生CO 2离解的不同条件和时间尺度,评估了不同碰撞过程的重要性。详细讨论了振动-平移温度比在不同条件下的长时间行为。结果表明,气体温度升高时的行为可以拟合为包含Landau-Teller温度依赖性的表达式。通过调整后的平均值来确认在低气体温度下,R平方值大于0.99,平均均方根误差值小于0.22。还讨论了拟合表达式的局限性,特别是条件和时间尺度,在该条件和时间尺度上可以产生更好的结果。
更新日期:2019-09-21
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