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N2 oxidation kinetics in a ns-pulsed discharge above a liquid electrode

Mikhail Gromov (UGent) , Kseniia Leonova, Nathalie De Geyter (UGent) , Rino Morent (UGent) , Rony Snyders, Nikolay Britun and Anton Nikiforov (UGent)
(2021) PLASMA SOURCES SCIENCE & TECHNOLOGY. 30(6).
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Abstract
In this work, the kinetics of nitrogen fixation via plasma-induced N-2 oxidation in a 10 ns pulsed atmospheric pressure water-contacting discharge sustained in air is investigated. Two pulse regimes, a single pulse and a three-pulse burst of 100 kHz, are considered. The densities of relevant radicals (NO, O) are studied by time- and space-resolved laser-induced fluorescence spectroscopy. It is concluded that in a single pulse mode, O atoms are mainly generated by O-2 reacting with electronically excited states of N-2 (A(3)Sigma(+)(u), B-3 Pi(g), C-3 Pi(u)) and are primarily reduced as a result of O-3 formation. The O density shows a maximum at similar to 100 ns after the plasma pulse with number density of similar to 10(23) m(-3). NO radicals, on the other hand, are primarily formed by reacting with the N-2(A(3)Sigma(+)(u)) state (up to similar to 1 mu s after the pulse) and with OH radicals (up to similar to 10's of mu s), peaking at approximately 60 mu s with a peak density of similar to 10(21) m(-3). The NO loss pathway is represented by the reversed Zeldovich mechanism at short time delays (similar to 10's mu s), whereas at longer delays (>100's of mu s) HNO2 and NO2 formation causing NO loss start to be dominant. In the burst mode, the energy efficiency of NO formation decreases despite higher N-2 conversion, for which three reasons are suggested: (1) NO removal by the generated O(D-1) after the discharge pulse through the reverse Zeldovich mechanism, (2) NO oxidation via the accumulated O-3, (3) pre-ionization induced by high pulse repetition rate (100 kHz) leading to shrinkage of the plasma bulk.
Keywords
Condensed Matter Physics, nitrogen fixation, laser-induced fluorescence spectroscopy, reactive oxygen and nitrogen species, nanosecond pulsed discharge, liquid electrode, INDUCED FLUORESCENCE SPECTROSCOPY, DENSITY-MEASUREMENTS, NO, NITROGEN, AIR

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Citation

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MLA
Gromov, Mikhail, et al. “N2 Oxidation Kinetics in a Ns-Pulsed Discharge above a Liquid Electrode.” PLASMA SOURCES SCIENCE & TECHNOLOGY, vol. 30, no. 6, 2021, doi:10.1088/1361-6595/abff71.
APA
Gromov, M., Leonova, K., De Geyter, N., Morent, R., Snyders, R., Britun, N., & Nikiforov, A. (2021). N2 oxidation kinetics in a ns-pulsed discharge above a liquid electrode. PLASMA SOURCES SCIENCE & TECHNOLOGY, 30(6). https://doi.org/10.1088/1361-6595/abff71
Chicago author-date
Gromov, Mikhail, Kseniia Leonova, Nathalie De Geyter, Rino Morent, Rony Snyders, Nikolay Britun, and Anton Nikiforov. 2021. “N2 Oxidation Kinetics in a Ns-Pulsed Discharge above a Liquid Electrode.” PLASMA SOURCES SCIENCE & TECHNOLOGY 30 (6). https://doi.org/10.1088/1361-6595/abff71.
Chicago author-date (all authors)
Gromov, Mikhail, Kseniia Leonova, Nathalie De Geyter, Rino Morent, Rony Snyders, Nikolay Britun, and Anton Nikiforov. 2021. “N2 Oxidation Kinetics in a Ns-Pulsed Discharge above a Liquid Electrode.” PLASMA SOURCES SCIENCE & TECHNOLOGY 30 (6). doi:10.1088/1361-6595/abff71.
Vancouver
1.
Gromov M, Leonova K, De Geyter N, Morent R, Snyders R, Britun N, et al. N2 oxidation kinetics in a ns-pulsed discharge above a liquid electrode. PLASMA SOURCES SCIENCE & TECHNOLOGY. 2021;30(6).
IEEE
[1]
M. Gromov et al., “N2 oxidation kinetics in a ns-pulsed discharge above a liquid electrode,” PLASMA SOURCES SCIENCE & TECHNOLOGY, vol. 30, no. 6, 2021.
@article{8736655,
  abstract     = {{In this work, the kinetics of nitrogen fixation via plasma-induced N-2 oxidation in a 10 ns pulsed atmospheric pressure water-contacting discharge sustained in air is investigated. Two pulse regimes, a single pulse and a three-pulse burst of 100 kHz, are considered. The densities of relevant radicals (NO, O) are studied by time- and space-resolved laser-induced fluorescence spectroscopy. It is concluded that in a single pulse mode, O atoms are mainly generated by O-2 reacting with electronically excited states of N-2 (A(3)Sigma(+)(u), B-3 Pi(g), C-3 Pi(u)) and are primarily reduced as a result of O-3 formation. The O density shows a maximum at similar to 100 ns after the plasma pulse with number density of similar to 10(23) m(-3). NO radicals, on the other hand, are primarily formed by reacting with the N-2(A(3)Sigma(+)(u)) state (up to similar to 1 mu s after the pulse) and with OH radicals (up to similar to 10's of mu s), peaking at approximately 60 mu s with a peak density of similar to 10(21) m(-3). The NO loss pathway is represented by the reversed Zeldovich mechanism at short time delays (similar to 10's mu s), whereas at longer delays (>100's of mu s) HNO2 and NO2 formation causing NO loss start to be dominant. In the burst mode, the energy efficiency of NO formation decreases despite higher N-2 conversion, for which three reasons are suggested: (1) NO removal by the generated O(D-1) after the discharge pulse through the reverse Zeldovich mechanism, (2) NO oxidation via the accumulated O-3, (3) pre-ionization induced by high pulse repetition rate (100 kHz) leading to shrinkage of the plasma bulk.}},
  articleno    = {{065024}},
  author       = {{Gromov, Mikhail and Leonova, Kseniia and De Geyter, Nathalie and Morent, Rino and Snyders, Rony and Britun, Nikolay and Nikiforov, Anton}},
  issn         = {{0963-0252}},
  journal      = {{PLASMA SOURCES SCIENCE & TECHNOLOGY}},
  keywords     = {{Condensed Matter Physics,nitrogen fixation,laser-induced fluorescence spectroscopy,reactive oxygen and nitrogen species,nanosecond pulsed discharge,liquid electrode,INDUCED FLUORESCENCE SPECTROSCOPY,DENSITY-MEASUREMENTS,NO,NITROGEN,AIR}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{14}},
  title        = {{N2 oxidation kinetics in a ns-pulsed discharge above a liquid electrode}},
  url          = {{http://doi.org/10.1088/1361-6595/abff71}},
  volume       = {{30}},
  year         = {{2021}},
}
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