1. A rotational Raman study under non-thermal conditions in pulsed CO2-N-2 and CO2-O-2 glow discharges
- Author
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Bart Klarenaar, Vasco Guerra, M. Grofulović, Olivier Guaitella, Rah Richard Engeln, Laboratoire de Physique des Plasmas (LPP), Université Paris-Saclay-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Université Paris-Sud - Paris 11 (UP11)-École polytechnique (X)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL), Plasma & Materials Processing, and Plasma-based gas conversion
- Subjects
010302 applied physics ,Glow discharge ,Materials science ,Analytical chemistry ,Rotational temperature ,02 engineering and technology ,rotational Raman spectroscopy ,glow discharge ,021001 nanoscience & nanotechnology ,Condensed Matter Physics ,vibrational excitation ,7. Clean energy ,01 natural sciences ,Dissociation (chemistry) ,Plasma current ,symbols.namesake ,[PHYS.PHYS.PHYS-PLASM-PH]Physics [physics]/Physics [physics]/Plasma Physics [physics.plasm-ph] ,0103 physical sciences ,Thermal ,symbols ,Total pressure ,Spatial homogeneity ,carbon dioxide plasma ,0210 nano-technology ,Raman spectroscopy - Abstract
International audience; This work employs in situ rotational Raman spectroscopy to study the effect of N2 and O2 addition to CO2 in pulsed glow discharges in the mbar range. The spatiotemporally resolved measurements are performed in CO2 and 25%, 50% and 75% of N2 or O2 admixture, in a 510 ms on-off cycle, 50 mA plasma current and 6.7 mbar total pressure. The rotational temperature profile is not affected by adding N2, ranging from 400 to 850 K from start to end of the discharge pulse, while the addition of O2 decreases the temperature at corresponding time points. Molecular number densities of CO2, CO, O2 and N2 are determined, showing the spatial homogeneity along the axis of the reactor and uniformity during the cycle. The measurements in the N2 containing mixtures show that CO2 conversion factor α increases from 0.15 to 0.33 when the content of N2 is increased from 0% to 75%, demonstrating the potential of N2 addition to enhance the vibrational pumping of CO2 and its beneficial effect on CO2 dissociation. Furthermore, the influence of admixtures on CO2 vibrations is examined by analysing the vibrationally averaged nuclear spin degeneracy. The difference between the fitted odd averaged degeneracy and the calculated odd degeneracy assuming thermal conditions increases with the addition of N2, demonstrating the growth of vibrational temperatures in CO2. On the other hand, the addition of O2 leads to a decrease of α, which might be attributed to quenched vibrations of CO2, and/or to the influence of the back reaction in the presence of O2.
- Published
- 2019
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