Effect of a pulsed high-current discharge on hydrogen-air mixtures

A self-consistent model describing the influence of a pulsed discharge on H₂-air mixtures is developed. The model includes the processes of ionization, dissociation, and excitation of the gas molecules by electron impacts; a set of ion-molecular reactions determining the time evolution of the charged particle densities; the processes involving electronically excited atoms and molecules; and a set of reactions describing the ignition of hydrogen-oxygen mixtures. Results are presented from simulations of the oxidation dynamics of hydrogen molecules in a stoichiometric H₂-air mixture and the ignition of such a mixture under the action of a pulsed high-current discharge. The simulation results are compared with available experimental data and calculations performed by other authors.     

Simulation of the ignition of a methane-air mixture by a high-voltage nanosecond discharge

The ignition dynamics of a CH₄: O₂: N₂: Ar = 1: 4: 15: 80 mixture by a high-voltage nanosecond discharge is simulated numerically with allowance for experimental data on the dynamics of the discharge current and discharge electric field. The calculated induction time agrees well with experimental data. It is shown that active particles produced in the discharge at a relatively low deposited energy can reduce the induction time by two orders of magnitude. Comparison of simulation results for mixtures with and without nitrogen shows that addition of nitrogen to the mixture leads to a decrease in the average electron energy in the discharge and gives rise to new mechanisms for accumulation of oxygen atoms due to the excitation of nitrogen electronic states and their subsequent quenching in collisions with oxygen molecules. Acceleration of the discharge-initiated ignition is caused by a faster initiation of chain reactions due to the production of active particles, first of all oxygen atoms, in the discharge.     

Ignition of a combustible gas mixture by a laser spark excited in the reactor volume

Ignition of a stoichiometric CH₄: O₂ mixture by a laser spark excited in the reactor volume is studied experimentally. It is found that the spark initiates a feebly radiating incomplete-combustion wave, which is much faster than the combustion wave, but is substantially slower than the detonation wave. With a time delay of 500–700 μs, a bright optical flash occupying the entire chamber volume is observed, which indicates fast (involving branching chain reactions) ignition of the gas mixture. A conclusion is drawn regarding the common nature of the process of ignition of a combustible gas mixture by a laser spark excited in the reactor volume and the previously investigated initiation of combustion by laser sparks excited at solid targets, high-power microwave discharges, and high-current gliding discharges.     

Combustion of methane-oxygen and methane-oxygen-CFC mixtures initiated by a high-current slipping surface discharge

Results are presented from experimental studies of the destruction of chlorofluorocarbon (CF₂Cl₂) molecules in a methane-oxygen (air) gas mixture whose combustion is initiated by a high-current slipping surface discharge. It is found that a three-component CH₄+O₂(air)+CF₂Cl₂ gas mixture (even with a considerable amount of the third component) demonstrates properties of explosive combustion involving chain reactions that are typical of two-component CH₄+O₂ mixtures. Experiments show the high degree of destruction (almost complete decomposition) of chlorofluorocarbons contained in the mixture during one combustion event. The combustion dynamics is studied. It is shown that the combustion initiated by a slipping surface discharge has a number of characteristic features that make it impossible to identify the combustion dynamics with the formation of a combustion or detonation wave. The features of the effects observed can be related to intense UV radiation produced by a pulsed high-current surface discharge.     

Alternating nonsteady gas-discharge modes in an atmospheric-pressure air flow blown through a point-plane gap

The electric and spectral characteristics of a nonsteady discharge in an atmospheric air flow blown through a point-plane interelectrode gap were investigated experimentally. The discharge was produced by applying a constant positive voltage to the point electrode, the amplitude of the applied voltage being much higher than the corona ignition voltage. The nonsteady character of the discharge is due to the spontaneously repeating streamer-spark breakdown, followed by the formation of either a diffuse ultracorona or a filamentary glow discharge. In the latter case, the length of the plasma column increases progressively, being blown off by the gas flow from the discharge gap. The extinction of a filamentary discharge is unrelated to the break of the current channel: the discharge decays abruptly when the filament length reaches its critical value. The distribution of active particles (O, OH, and N*₂) carried out from the discharge gap is determined from the data of spectral measurements.     

Effect of a small C3O2 additive on the vibrational distribution function of CO molecules in a low-temperature plasma

The concentration of carbon suboxide (C₃O₂) in the plasmas of sealed-off discharges in mixtures of CO with noble gases is measured for the first time by mass-spectroscopic technique. It is shown that the production of C₃O₂ (and, possibly, more complex carbon oxides) in a gas-discharge plasma significantly boosts the vibrational relaxation of CO molecules and thus greatly affects their vibrational populations. Adding xenon to a He: CO mixture reduces the concentration of C₃O₂. The effect of pulsed UV radiation on the vibrational populations of CO molecules is studied experimentally. It is shown that UV irradiation of the gas mixture after long-term discharge operation increases vibrational populations in the plateau region up to the values observed at the beginning of the discharge. This effect is attributed to the decay of C₃O₂ molecules under the action of UV radiation.     

Electrical and chemical properties of XeCl*(308 nm) exciplex lamp created by a dielectric barrier discharge

The aim of this work is to highlight, through numerical modeling, the chemical and the electrical characteristics of xenon chloride mixture in XeCl* (308 nm) excimer lamp created by a dielectric barrier discharge. A temporal model, based on the Xe/Cl₂ mixture chemistry, the circuit and the Boltzmann equations, is constructed. The effects of operating voltage, Cl₂ percentage in the Xe/Cl₂ gas mixture, dielectric capacitance, as well as gas pressure on the 308-nm photon generation, under typical experimental operating conditions, have been investigated and discussed. The importance of charged and excited species, including the major electronic and ionic processes, is also demonstrated. The present calculations show clearly that the model predicts the optimal operating conditions and describes the electrical and chemical properties of the XeCl* exciplex lamp.     

Simulation of toluene decomposition in a pulse-periodic discharge operating in a mixture of molecular nitrogen and oxygen

The kinetic model of toluene decomposition in nonequilibrium low-temperature plasma generated by a pulse-periodic discharge operating in a mixture of nitrogen and oxygen is developed. The results of numerical simulation of plasma-chemical conversion of toluene are presented; the main processes responsible for C₆H₅CH₃ decomposition are identified; the contribution of each process to total removal of toluene is determined; and the intermediate and final products of C₆H₅CH₃ decomposition are identified. It was shown that toluene in pure nitrogen is mostly decomposed in its reactions with metastable N₂(A₃?? _u ⁺ ) and N₂(a??¹?? _u ^? ) molecules. In the presence of oxygen, in the N₂ : O₂ gas mixture, the largest contribution to C₆H₅CH₃ removal is made by the hydroxyl radical OH which is generated in this mixture exclusively due to plasma-chemical reactions between toluene and oxygen decomposition products. Numerical simulation showed the existence of an optimum oxygen concentration in the mixture, at which toluene removal is maximum at a fixed energy deposition.     

Influence of a Nitrogen Admixture on the Anomalous Memory Effect in the Breakdown of Low-Pressure Argon in a Long Discharge Tube

The memory effect (the dependence of the dynamic breakdown voltage U _b on the time interval τ between voltage pulses) in pulse-periodic discharges in pure argon and the Ar + 1%N₂ mixture was studied experimentally. The discharge was ignited in a 2.8-cm-diameter tube with an interelectrode distance of 75 cm. The measurements were performed at gas pressures of P = 1, 2, and 5 Torr and discharge currents in a steady stage of the discharge of I = 20 and 56 mA. Breakdown was produced by applying positive-polarity voltage pulses, the time interval between pulses being in the range of τ = 0.5–40 ms. In this range of τ values, a local maximum (the anomalous memory effect) was observed in the dependence U _b (τ). It is shown that addition of nitrogen to argon substantially narrows the range of τ values at which this effect takes place. To analyze the measurement results, the plasma parameters in a steady-state discharge (in both pure argon and the Ar + 1%N₂ mixture) and its afterglow were calculated for the given experimental conditions. Analysis of the experimental data shows that the influence of the nitrogen admixture on the shape of the dependence U _b (τ) is, to a large extent, caused by the change in the decay rate of the argon afterglow plasma in the presence of a nitrogen admixture.     

Polycrystal diamond growth in a microwave plasma torch

Diamond films of different structures were deposited on quartz, WC-Co, and molybdenum substrates in a microwave plasma torch discharge in an argon-hydrogen-methane gas mixture in a sealed chamber at pressures close to atmospheric by using the chemical vapor deposition technique. Images of diamond polycrystal films and separate crystals, as well as results of Raman spectroscopy, are presented. The spectra of optical plasma radiation recorded during film deposition demonstrate the presence of intense H_α hydrogen and C₂ radical bands known as Swan bands.     

Plasma kinetics of ethanol conversion in a glow discharge

The mechanism of ethanol conversion in a nonequilibrium glow discharge has been studied. It is shown that molecular hydrogen is produced in reactions between ethanol molecules and hydrogen atoms in the initial stage and in reactions involving active H, CH₂OH, CH₃CHOH, and formaldehyde in the final stage. Comparison with experimental data shows that the kinetic mechanism used in these calculations correctly predicts the concentrations of the main components of the gas mixture.     

Decomposition of toluene in a steady-state atmospheric-pressure glow discharge

Results are presented from experimental studies of decomposition of toluene (C₆H₅CH₃) in a polluted air flow by means of a steady-state atmospheric pressure glow discharge at different water vapor contents in the working gas. The experimental results on the degree of C₆H₅CH₃ removal are compared with the results of computer simulations conducted in the framework of the developed kinetic model of plasma chemical decomposition of toluene in the N₂: O₂: H₂O gas mixture. A substantial influence of the gas flow humidity on toluene decomposition in the atmospheric pressure glow discharge is demonstrated. The main mechanisms of the influence of humidity on C₆H₅CH₃ decomposition are determined. The existence of two stages in the process of toluene removal, which differ in their duration and the intensity of plasma chemical decomposition of C₆H₅CH₃ is established. Based on the results of computer simulations, the composition of the products of plasma chemical reactions at the output of the reactor is analyzed as a function of the specific energy deposition and gas flow humidity. The existence of a catalytic cycle in which hydroxyl radical OH acts a catalyst and which substantially accelerates the recombination of oxygen atoms and suppression of ozone generation when the plasma-forming gas contains water vapor is established.     

Influence of the chlorine concentration on the radiation efficiency of a XeCl exciplex lamp

The influence of the chlorine concentration on the radiation efficiency of coaxial exciplex lamps (excilamps) excited by a dielectric barrier discharge (DBD) in binary Xe-Cl₂ mixtures at pressures of 240–250 Torr is investigated experimentally and theoretically. The experiments were carried out at Cl₂ concentrations in the range of 0.01–1%. The DBD characteristics were calculated in the framework of a one-dimensional hydrodynamic model at Cl₂ concentrations in the range of 0.1–5%. It is found that the radiation intensities of the emission bands of Xe*₂(172 nm) and XeCl* (308 nm) are comparable when the chlorine concentration in the mixture is in the range of 0.01–0.1%. In this case, in the mixture, the radiation intensity of the Xe*₂ molecule rapidly decreases with increasing Cl₂ concentration and, at a chlorine concentration of ≥0.2%, the radiation of the B → X band of XeCl* molecules with a peak at 308 nm dominates in the discharge radiation. The radiation efficiency of this band reaches its maximum value at chlorine concentrations in the range of 0.4–0.5%. The calculated efficiencies of DBD radiation exceed those obtained experimentally. This is due to limitations of the one-dimensional model, which assumes the discharge to be uniform in the transverse direction, whereas the actual excilamp discharge is highly inhomogeneous. The influence of the chlorine concentration on the properties of the DBD plasma in binary Xe-Cl₂ mixtures is studied numerically. It is shown that an increase in the Cl₂ concentration in the mixture leads to the attachment of electrons to chlorine atoms and a decrease in the electron density and discharge conductivity. As a result, the electric field and the voltage drop across the discharge gap increase, which, in turn, leads to an increase in the average electron energy and the probability of dissociation of Cl₂ molecules and ionization of Xe atoms and Cl₂ molecules. The total energy deposited in the discharge rises with increasing chlorine concentration due to an increase in the power spent on the heating of positive and negative ions. The power dissipated by electrons decreases with increasing chlorine concentration in the working mixture. Recommendations on the choice of the chlorine content in the mixture for reducing the intensity of VUV radiation of the second continuum of the Xe*₂ excimer without a substantial decrease in the excilamp efficiency are formulated.     

Production of singlet oxygen in a non-self-sustained discharge

The production of O₂(a¹Δ_g) singlet oxygen in non-self-sustained discharges in pure oxygen and mixtures of oxygen with noble gases (Ar or He) was studied experimentally. It is shown that the energy efficiency of O₂(a¹Δ_g production can be optimized with respect to the reduced electric field E/N. It is shown that the optimal E/N values correspond to electron temperatures of 1.2–1.4 eV. At these E/N values, a decrease in the oxygen percentage in the mixture leads to an increase in the excitation rate of singlet oxygen because of the increase in the specific energy deposition per O₂ molecule. The onset of discharge instabilities not only greatly reduces the energy efficiency of singlet oxygen production but also makes it impossible to achieve high energy deposition in a non-self-sustained discharge. A model of a non-self-sustained discharge in pure oxygen is developed. It is shown that good agreement between the experimental and computed results for a discharge in oxygen over a wide range of reduced electric fields can be achieved only by taking into account the ion component of the discharge current. The cross section for the electron-impact excitation of O₂(a¹Δ_g and the kinetic scheme of the discharge processes with the participation of singlet oxygen are verified by comparing the experimental and computed data on the energy efficiency of the production of O₂(a¹Δ_g and the dynamics of its concentration. It is shown that, in the dynamics of O₂(a¹Δ_g molecules in the discharge afterglow, an important role is played by their deexcitation in a three-body reaction with the participation of O(³P) atoms. At high energy depositions in a non-self-sustained discharge, this reaction can reduce the maximal attainable concentration of singlet oxygen. The effect of a hydrogen additive to an Ar: O₂ mixture is analyzed based on the results obtained using the model developed. It is shown that, for actual electron beam current densities, a significant energy deposition in a non-self-sustained discharge in the mixtures under study can be achieved due to the high rate of electron detachment from negative ions. In this case, however, significant heating of the mixture can lead to a rapid quenching of O₂(a¹Δ_g molecules by atomic hydrogen.     

Effect of hydrogen ratio on plasma parameters of N2-H2 gas mixture glow discharge

A dc plane glow discharge in a nitrogen-hydrogen (N₂-H₂) gas mixture has been operated at discharge currents of 10 and 20 mA. The electron energy distribution function (EEDF) at different hydrogen concentrations is measured. A Maxwellian EEDF is found in the positive column region, while in both cathode fall and negative glow regions, a non-Maxwellian one is observed. Langmuir electric probes are used at different axial positions, gas pressures, and hydrogen concentrations to measure the electron temperature and plasma density. The electron temperature is found to increase with increasing H₂ concentration and decrease with increasing both the axial distance from the cathode and the mixture pressure. At first, with increasing distance from the cathode, the ion density decreases, while the electron density increases; then, as the anode is further approached, they remain nearly constant. At different H₂ concentrations, the electron and ion densities decrease with increasing the mixture pressure. Both the electron and ion densities slightly decrease with increasing H₂ concentration.     

Characteristics of a transverse RF discharge in Xe/Cl<Subscript>2</Subscript> mixtures

Results are presented from the study of the electrical and optical characteristics of a transverse RF discharge in Xe/Cl₂ mixtures at pressures of p≤400 Pa. The working mixture was excited by a modulated RF discharge (f=1.76 MHz) with a transverse electrode configuration (L≤17 cm). The emission spectrum in the spectral range of 210–600 nm and the waveforms of the discharge current, discharge voltage, and plasma emission intensity were investigated. The UV emission power from the discharge was studied as a function of the pressure and composition of a Xe/Cl₂ mixture. It is shown that a discharge in a xenon-chlorine mixture acts as planar excimer-halogen lamp operating in the spectral range of 220–450 nm, which contains a system of overlapping XeCl(D, B-X; B, C-A) and Cl₂(D′-A′) bands. Transverse RF discharges in Xe/Cl₂ mixtures can be used to create a wideband lamp with two 50-cm² planar apertures and the low circulation rate of the working mixture.     

Simulation of ethylene conversion initiated by a streamer corona in an air flow

The conversion of ethylene (C₂H₄) at concentrations of 400 and 930 ppm in an air flow at a temperature of 295 K is simulated. Ethylene is added to air either upstream of the discharge chamber or in the reaction tube, downstream of a pulsed corona discharge. It is taken into account that the distribution of the gas components in the discharge zone is nonuniform due to the streamer nature of the discharge. In the reaction tube, all of the components are assumed to be uniform. Simulation results agree with the experiments carried out at voltage pulse amplitudes of 30 and 40 kV, a gas flow rate of 2–10 l/min, and a specific energy deposition of up to 0.15 J/cm³. It is shown that the ozone produced plays a governing role in the C₂H₄ conversion. It is found that it is possible to minimize the energy spent on conversion by choosing the optimum pulse repetition rate and the specific energy deposited per pulse. The presence of water vapor impedes the ethylene conversion and increases the concentration of formaldehyde and methane.     

Simulations of a longitudinal glow discharge in a hot air flow at atmospheric pressure

A one-dimensional axisymmetric time-dependent model of a discharge in a gas flow is developed. The model includes a fairly complete set of plasmochemical reactions and describes the heating and gasdynamic expansion of a plasma channel in air. The processes governing the distribution of nitrogen molecules in the N₂(C ³Π_u, v) state over vibrational levels are considered. The parameters of a longitudinal glow discharge in a hot (T ₀ = 1500?3000 K) air flow at atmospheric pressure are calculated. It is found that gas preheating considerably influences the parameters of the discharge channel. The results of calculations are compared with the experimental data.     

Modeling of a Ne/Xe dielectric barrier discharge excilamp for improvement of VUV radiation production

This work is devoted to excimer lamp efficiency optimization by using a homogenous discharge model of a dielectric barrier discharge in a Ne?Xe mixture. The model includes the plasma chemistry, electrical circuit, and Boltzmann equation. In this paper, we are particularly interested in the electrical and kinetic properties and light output generated by the DBD. Xenon is chosen for its high luminescence in the range of vacuum UV radiation around 173 nm. Our study is motivated by interest in this type of discharge in many industrial applications, including the achievement of high light output lamps. In this work, we used an applied sinusoidal voltage, frequency, gas pressure, and concentration in the ranges of 2–8 kV, 10–200 kHz, 100–800 Torr, and 10–50%, respectively. The analyzed results concern the voltage V _p across the gap, the dielectric voltage V _d, the discharge current I, and the particles densities. We also investigated the effect of the electric parameters and xenon concentration on the lamp efficiency. This investigation will allow one to find out the appropriate parameters for Ne/Xe DBD excilamps to improve their efficiency.