Two-temperature model of the non-thermal chemical dissociation of CO2†

IF 3.4 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Q. Shen, A. Pikalev, F. J. J. Peeters, J. Gans and M. C. M. van de Sanden
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Abstract

A two-temperature model with a vibrational temperature different from the gas temperature is presented for the decomposition of CO2. All vibrational modes of CO2, CO and O2 are included, and a novel procedure to calculate the vibrational–dissociation reaction rate constant is proposed. In all cases, a Boltzmann distribution is assumed for the vibrational states and the effect of the activation barrier on the chemical reactions is taken into account using the Fridman–Macheret expression. The non-thermal reaction rate constants are therefore functions of gas and vibrational temperatures. The results show that relatively higher vibrational temperatures benefit CO2 conversion. This work provides more insights into the dissociation and recombination reactions of CO2 conversion under non-thermal conditions and offers the opportunity for multi-dimensional non-thermal modelling in the future.

Abstract Image

CO2†非热化学解离的双温模型
提出了一种振动温度与气体温度不同的CO2分解双温模型。考虑了CO2、CO和O2的所有振动模式,提出了一种计算振动解离反应速率常数的新方法。在所有情况下,假设振动态为玻尔兹曼分布,并且使用弗里德曼-马赫雷表达式考虑了激活势垒对化学反应的影响。因此,非热反应速率常数是气体温度和振动温度的函数。结果表明,较高的振动温度有利于CO2的转化。这项工作为非热条件下CO2转化的解离和重组反应提供了更多的见解,并为未来的多维非热建模提供了机会。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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