Edmond Baratte, Carolina A. Garcia-Soto, Tiago Silva, Vasco Guerra, Vasile I. Parvulescu, Olivier Guaitella
{"title":"$$\\hbox {CO}_2$$ / $$\\hbox {CH}_4$$辉光放电等离子体:第一部分-反应途径的实验和数值研究","authors":"Edmond Baratte, Carolina A. Garcia-Soto, Tiago Silva, Vasco Guerra, Vasile I. Parvulescu, Olivier Guaitella","doi":"10.1007/s11090-023-10421-z","DOIUrl":null,"url":null,"abstract":"<p>A fundamental study of <span>\\(\\hbox {CO}_2\\)</span>/<span>\\(\\hbox {CH}_4\\)</span> plasma is performed in a glow discharge at a few Torr. Experimental and numerical results are compared to identify the main reaction pathways. OES-based techniques and FTIR (Fourier Transform Infrared) spectroscopy are used to determine molecules densities and gas temperature. Several conditions of pressure, initial mixture and residence time are measured. The main dissociation products are found to be CO and <span>\\(\\hbox {H}_2\\)</span>. The LoKI simulation tool was used to build a simplified kinetic scheme to limit the uncertainties on rate coefficients, but sufficient to reproduce the experimental data. To this aim, only molecules containing at most one carbon atom are considered based on the experimental observations. Obtaining a good match between the experimental data and the simulation requires the inclusion of reactions involving the excited state <span>\\(\\hbox {O}(^{1}\\hbox {D})\\)</span>. The key role of <span>\\(\\hbox {CH}_3\\)</span> radical is also emphasized. The good match obtained between the experiment and the simulation allows to draw the main reaction pathways of the low-pressure <span>\\(\\hbox {CO}_2\\)</span>-<span>\\(\\hbox {CH}_4\\)</span> plasmas, in particular to identify the main back reaction mechanisms for <span>\\(\\hbox {CO}_2\\)</span>. The role of <span>\\(\\hbox {CH}_2\\)</span>O and <span>\\(\\hbox {H}_2\\)</span>O in the gas phase is also discussed in depth as they appear to play an important role on catalytic surface studied in the part II of this study.\n</p>","PeriodicalId":734,"journal":{"name":"Plasma Chemistry and Plasma Processing","volume":null,"pages":null},"PeriodicalIF":2.6000,"publicationDate":"2023-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"$$\\\\hbox {CO}_2$$ / $$\\\\hbox {CH}_4$$ Glow Discharge Plasma: Part I—Experimental and Numerical Study of the Reaction Pathways\",\"authors\":\"Edmond Baratte, Carolina A. Garcia-Soto, Tiago Silva, Vasco Guerra, Vasile I. 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$$\hbox {CO}_2$$ / $$\hbox {CH}_4$$ Glow Discharge Plasma: Part I—Experimental and Numerical Study of the Reaction Pathways
A fundamental study of \(\hbox {CO}_2\)/\(\hbox {CH}_4\) plasma is performed in a glow discharge at a few Torr. Experimental and numerical results are compared to identify the main reaction pathways. OES-based techniques and FTIR (Fourier Transform Infrared) spectroscopy are used to determine molecules densities and gas temperature. Several conditions of pressure, initial mixture and residence time are measured. The main dissociation products are found to be CO and \(\hbox {H}_2\). The LoKI simulation tool was used to build a simplified kinetic scheme to limit the uncertainties on rate coefficients, but sufficient to reproduce the experimental data. To this aim, only molecules containing at most one carbon atom are considered based on the experimental observations. Obtaining a good match between the experimental data and the simulation requires the inclusion of reactions involving the excited state \(\hbox {O}(^{1}\hbox {D})\). The key role of \(\hbox {CH}_3\) radical is also emphasized. The good match obtained between the experiment and the simulation allows to draw the main reaction pathways of the low-pressure \(\hbox {CO}_2\)-\(\hbox {CH}_4\) plasmas, in particular to identify the main back reaction mechanisms for \(\hbox {CO}_2\). The role of \(\hbox {CH}_2\)O and \(\hbox {H}_2\)O in the gas phase is also discussed in depth as they appear to play an important role on catalytic surface studied in the part II of this study.
期刊介绍:
Publishing original papers on fundamental and applied research in plasma chemistry and plasma processing, the scope of this journal includes processing plasmas ranging from non-thermal plasmas to thermal plasmas, and fundamental plasma studies as well as studies of specific plasma applications. Such applications include but are not limited to plasma catalysis, environmental processing including treatment of liquids and gases, biological applications of plasmas including plasma medicine and agriculture, surface modification and deposition, powder and nanostructure synthesis, energy applications including plasma combustion and reforming, resource recovery, coupling of plasmas and electrochemistry, and plasma etching. Studies of chemical kinetics in plasmas, and the interactions of plasmas with surfaces are also solicited. It is essential that submissions include substantial consideration of the role of the plasma, for example, the relevant plasma chemistry, plasma physics or plasma–surface interactions; manuscripts that consider solely the properties of materials or substances processed using a plasma are not within the journal’s scope.