Time-resolved CO 2 , CO, and N 2 vibrational population measurements in Ns pulse discharge plasmas

Richards, Caleb; Jans, Elijah; Mignogna, David; Adamovich, Igor V.

doi:10.1088/1361-6595/ac8f6d

Time-resolved CO ₂ , CO, and N ₂ vibrational population measurements in Ns pulse discharge plasmas

Journal Article · Thu Sep 01 00:00:00 EDT 2022 · Plasma Sources Science and Technology

DOI:https://doi.org/10.1088/1361-6595/ac8f6d· OSTI ID:1982448

; ; Mignogna, David;

Abstract

Time-resolved CO₂and N₂vibrational populations and translational-rotational temperature are measured in a CO₂–N₂plasma sustained by a ns pulse discharge burst in plane-to-plane geometry. Time-resolved, absolute number density of CO generated in the plasma is also inferred from the experimental data. CO₂and CO vibrational populations are measured by mid-IR, tunable quantum cascade laser absorption spectroscopy, and N₂vibrational populations are measured by the ns broadband vibrational CARS. Transient excitation of N₂and CO₂asymmetric stretch vibrational energy modes is detected during the discharge burst. The time-resolved rate of CO generation does not correlate with N₂or CO₂(ν₃) vibrational temperatures, indicating that CO₂dissociation via the vibrational excitation is insignificant at the present conditions. The rate of CO generation decreases gradually during the discharge burst. The estimated specific energy cost of the CO product is close to that of N atoms in pure nitrogen, measured previously at similar operating conditions. Comparison of the experimental data with the kinetic modeling analysis indicates that CO₂dissociation in collisions with electronically excited N₂molecules is the dominant channel of CO generation at the present conditions, although the inferred CO yield in these processes is significantly lower than 1. The effect of vibrational energy transfer between N₂and CO₂on the plasma chemical processes is insignificant. The kinetic model underpredicts a rapid reduction of the N₂and CO₂(ν₃) vibrational temperatures during the later half of the discharge burst and in the afterglow. V–T relaxation of N₂by N and O atoms generated in the ns pulse discharge plasma does not affect the vibrational relaxation rate in a significant way. However, rapid V–T relaxation of CO₂by O atoms has a significant effect on the relaxation rate. The difference between the experimental data and the modeling predictions may be due to the unknown scaling of the CO₂–O V–T rates with the vibrational quantum number.

Research Organization:: The Ohio State Univ., Columbus, OH (United States)

Sponsoring Organization:: USDOE

OSTI ID:: 1982448

Journal Information:: Plasma Sources Science and Technology, Journal Name: Plasma Sources Science and Technology Journal Issue: 9 Vol. 31; ISSN 0963-0252

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

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