skip to main content


Title: Impact of CH 4 addition on the electron properties and electric field dynamics in a Ar nanosecond-pulsed dielectric barrier discharge
Abstract Non-equilibrium plasmas derive their low temperature reactivity from producing and driving energetic electrons and active species under large electric fields. Therefore, the impact of reactants on the plasma properties including electron number density, electric field, and electron temperature is critical for applications such as plasma methane (CH 4 ) reforming. Due to experimental complexity, electron properties and the electric field are rarely measured together in the same discharge. In this work, we combine time-resolved Thomson scattering and electric field induced second harmonic generation to probe electron temperature, electron density, and electric field strength in a 60 Torr CH 4 /Ar nanosecond-pulsed dielectric barrier discharge while varying the CH 4 mole fraction from 0% to 8%. These measurements are compared to a 1D numerical model to benchmark its predictions and identify areas of uncertainty. Nonlinear coupling between CH 4 addition, electron temperature, electron density, and the electric field was directly observed. Contrary to previous measurements in He, the electron temperature increased with CH 4 mole fraction. This rise in electron temperature is identified as electron heating by residual electric fields that increased with larger CH 4 mole fraction. Moreover, the electron number density has been found to decrease rapidly with the increase of methane mole fraction. Comparison of these measurements with the model yielded better agreement at higher CH 4 mole fractions and with the usage of ab initio calculated Ar electron-impact cross-sections from the B-spline R-matrix database. Furthermore, the calculated plasma properties are shown to be sensitive to the residual surface charge implanted on the quartz dielectric surfaces. Without considering surface charge in the simulations, the calculated electric field profiles agreed well with the measurements, but the electron properties were underpredicted by more than a factor of three. Therefore, measurements of either the electric field or electron properties measurements alone are insufficient to fully validate modeling predictions.  more » « less
Award ID(s):
2029425
PAR ID:
10465965
Author(s) / Creator(s):
; ; ; ; ; ; ;
Publisher / Repository:
Elsevier
Date Published:
Journal Name:
Plasma Sources Science and Technology
Volume:
31
Issue:
12
ISSN:
0963-0252
Page Range / eLocation ID:
125013
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Manipulating surface charge, electric field, and plasma afterglow in a non-equilibrium plasma is critical to control plasma-surface interaction for plasma catalysis and manufacturing. Here, we show enhancements of surface charge, electric field during breakdown, and afterglow by ferroelectric barrier discharge. The results show that the ferroelectrics manifest spontaneous electric polarization to increase the surface charge by two orders of magnitude compared to discharge with an alumina barrier. Time-resolved in-situ electric field measurements reveal that the fast polarization of ferroelectrics enhances the electric field during the breakdown in streamer discharge and doubles the electric field compared to the dielectric barrier discharge. Moreover, due to the existence of surface charge, the ferroelectric electrode extends the afterglow time and makes discharge sustained longer when alternating the external electric field polarity. The present results show that ferroelectric barrier discharge offers a promising technique to tune plasma properties for efficient plasma catalysis and electrified manufacturing.

     
    more » « less
  2. Abstract

    A nonthermal, pulsed spark discharge is applied to three polymer powders in Ar and Ar– gas mixtures. Hydrogen is introduced to assess plasma‐driven decomposition. Gaseous decomposition products, including methane, acetylene, and ethylene, are observed with Fourier‐transform infrared (FTIR). Surface modifications are observed on the residual polymer via attenuated total internal reflection‐FTIR. Time‐averaged rotational, vibrational, and excitation temperatures are characterized in the discharge. The plasma density is found to be around , with rotational and vibrational temperatures ranging from 1500 to 2200 K and an excitation temperature of 1–2 eV. While spark properties did not change with either gas composition or polymer composition, it was determined that the addition of hydrogen promoted higher concentrations of gaseous phase products (promoting hydrogenolysis).

     
    more » « less
  3. This paper presents the development and application of a broadband ultrafast-laser-absorption-spectroscopy (ULAS) technique operating in the mid-infrared for simultaneous measurements of temperature, methane (CH4), and propane (C3H8) mole fractions. Single-shot measurements targeting the C-H stretch fundamental vibration bands of CH4and C3H8near 3.3 µm were acquired in both a heated gas cell up to ≈650K and laminar diffusion flames at 5 kHz. The average temperature error is 0.6%. The average species mole fraction errors are 5.4% for CH4and 9.9% for C3H8. This demonstrates that ULAS is capable of providing high-fidelity hydrocarbon-based thermometry and simultaneous measurements of both large and small hydrocarbons in combustion gases.

     
    more » « less
  4. The conversion of methane, CH4, into higher value chemicals using low temperature plasmas is challenged by both improving efficiency and selectivity. One path towards selectivity is capturing plasma produced methyl radicals, CH3, in a solvent for aqueous processing. Due to the rapid reactions of methyl radicals in the gas phase, the transport distance from production of the CH3 to its solvation should be short, which then motivates the use of microplasmas. The generation of CH3 in Ar/CH4/H2O plasmas produced in nanosecond pulsed dielectric barrier discharge microplasmas is discussed using results from a computational investigation. The microplasma is sustained in the channel of a microfluidic chip in which the solvent flows along one wall or in droplets. CH3 is primarily produced by electron-impact of and dissociative excitation transfer to CH4, as well as CH2 reacting with CH4. CH3 is rapidly consumed to form C2H6 which, in spite of being subject to these same dissociative processes, accumulates over time, as do other stable products including C3H8 and CH¬3OH. The gas mixture and electrical properties were varied to assess their effects on CH3 production. CH3 production is largest with 5% CH4 in the Ar/CH4/H2O mixture due to an optimal balance of electron-impact dissociation, which increases with CH4 percentage, and dissociative excitation transfer and CH2 reacting with CH4, which decrease with CH4 percentage. Design parameters of the microchannels were also investigated. Increasing the permittivity of the dielectrics in contact with the plasma increased the ionization wave intensity which increased CH3 production. Increased energy deposition per pulse generally increased CH3 production as does lengthening pulse length up to a certain point. The arrangement of the solvent flow in the microchannel can also affect the CH3 density and fluence to the solvent. The fluence of CH3 to the liquid solvent is increased if the liquid is immersed in the plasma as a droplet or is a layer on the wall where the ionization wave terminates. The solvation dynamics of CH3 with varying numbers of droplets was also examined. The maximum density of solvated methyl radicals CH3aq occurs with a large number of droplets in the plasma. However, the solvated CH3aq density can rapidly decrease due to desolvation, emphasizing the need to quickly react the solvated species in the solvent. 
    more » « less
  5. Interactions at the interface between atmospheric pressure plasmas and liquids are being investigated to address applications ranging from nanoparticle synthesis to decontamination and fertilizer production. Many of these applications involve activation of droplets wherein the droplet is fully immersed in the plasma and synergistically interacts with the plasma. To better understand these interactions, two-dimensional modeling of radio frequency (RF) glow discharges at atmospheric pressure operated in He with an embedded lossy dielectric droplet (tens of microns in size) was performed. The properties of the sheath that forms around the droplet were investigated over the RF cycle. The electric field in the bulk plasma polarizes the dielectric droplet while the electron drift in the external electric field is shadowed by the droplet. The interaction between the bulk and sheath electric fields produces a maximum in E/N (electric field/gas number density) at the equator on one side of the droplet where the bulk and sheath fields are aligned in the same direction and a minimum along the opposite equator. Due to resistive heating, the electron temperature T e is maximum 45° above and below the equator of the droplet where power deposition per electron is the highest. Although the droplet is, on the average, negatively charged, the charge density on the droplet is positive on the poles and negative on the equator, as the electron motion is primarily due to diffusion at the poles but due to drift at the equator. 
    more » « less