Q. Shen, A. Pikalev, F. J. J. Peeters, J. Gans and M. C. M. van de Sanden
{"title":"Two-temperature model of the non-thermal chemical dissociation of CO2†","authors":"Q. Shen, A. Pikalev, F. J. J. Peeters, J. Gans and M. C. M. van de Sanden","doi":"10.1039/D4RE00300D","DOIUrl":null,"url":null,"abstract":"<p >A two-temperature model with a vibrational temperature different from the gas temperature is presented for the decomposition of CO<small><sub>2</sub></small>. All vibrational modes of CO<small><sub>2</sub></small>, CO and O<small><sub>2</sub></small> 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 CO<small><sub>2</sub></small> conversion. This work provides more insights into the dissociation and recombination reactions of CO<small><sub>2</sub></small> conversion under non-thermal conditions and offers the opportunity for multi-dimensional non-thermal modelling in the future.</p>","PeriodicalId":101,"journal":{"name":"Reaction Chemistry & Engineering","volume":" 1","pages":" 146-157"},"PeriodicalIF":3.4000,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Reaction Chemistry & Engineering","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/re/d4re00300d","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
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.
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.