A numerical simulation study on active species production in dense methane-air plasma discharge

Recently, low-temperature atmospheric pressure plasmas have been proposed as a potential type of ‘reaction carrier' for the conversion of methane into value-added chemicals. In this paper, the multi-physics field coupling software of COMSOL is used to simulate the detailed discharge characteristics of atmospheric pressure methane-air plasma. A two-dimensional axisymmetric fluid model is constructed, in which 77 plasma chemical reactions and 32 different species are taken into account. The spatial density distributions of dominant charged ions and reactive radical species, such as CH_4~+CH_3~+N_2~+O_2~+H, O, CH_3, and CH_2, are presented, which is due to plasma chemical reactions of methane/air dissociation(or ionization) and reforming of small fragment radical species. The physicochemical mechanisms of methane dissociation and radical species recombination are also discussed and analyzed.     

Investigation of NO removal using a pulse-assisted RF discharge

In this paper,removal of nitrogen oxide (NO) is investigated in capacitive atmospheric pressure discharges driven by both radio-frequency (RF) and trapezoidal pulsed power with a onedimensional self-consistent fluid model.The results show that the number density of NO could be reduced significantly once a short pulse of low duty ratio is additionally applied to the RF power.It is found that the process of NO removal by the pulse-modulated RF discharge could be divided into three stages:the quick reaction stage,the NO removal stage,and the sustaining stage.Furthermore,the temporal evolution of particle densities is analyzed,and the key reactions in each stage are discovered.Finally,the influence on the removal efficiency of the voltage amplitude of the pulse and the RF voltage amplitude is investigated.     

Effects of HF frequency on plasma characteristics in dual-frequency helium discharge at atmospheric pressure by fluid modeling

On the basis of the fluid theory and the drift–diffusion approximation, a numerical model for dual-frequency atmospheric pressure helium discharge is established, in order to investigate the effects of the high frequency source (HF) on the characteristics of dual-frequency atmospheric pressure helium discharge. The numerical results showed that the electron heating rate increases with enhancing HF frequency, as well as the particles densities, electron dissipation rate, current density, net electron generation and bulk plasma region. Moreover, it is also observed that the efficient electron heating region moves when the HF frequency has been changed. The plasma parameters are not linear change with the HF frequency linearly increasing.     

The double coupled microwave resonance probes and application for diagnosing atmospheric pressure plasma jet

The double-coupled microwave resonance probe(DMRP) based on the hairpin probe is proposed for diagnosing atmospheric plasma jet(n_e10~(17) m~(-3)). In this work, the resonance characteristics of DMRP are investigated by numerical simulation. It shows that two resonance peaks on the reflectance spectrum can be observed, and influenced significantly by some parameters, such as the probe separation, the distance to the handheld radio frequency atmospheric pressure glow discharge plasma jet(RF-APGDPJ) and the plasma electron density less than 1017 m~(-3). Based on two resonance modes of DMRP, the electron densities in the afterglow of RF-APGDPJ at the different rf powers and helium flow rates are diagnosed experimentally by matching the change of FWHM(Df_1-Df_(1,air)and Df_2-Df_(2,air)) measured by vector network analyzer with the simulated relation between the FWHM changes and the plasma density.     

Characteristics of Atmospheric Pressure Rotating Gliding Arc Plasmas

In this work,a novel direct current (DC) atmospheric pressure rotating gliding arc (RGA) plasma reactor has been developed for plasma-assisted chemical reactions.The influence of the gas composition and the gas flow rate on the arc dynamic behaviour and the formation of reactive species in the N2 and air gliding arc plasmas has been investigated by means of electrical signals,high speed photography,and optical emission spectroscopic diagnostics.Compared to conventional gliding arc reactors with knife-shaped electrodes which generally require a high flow rate (e.g.,10-20 L/min) to maintain a long arc length and reasonable plasma discharge zone,in this RGA system,a lower gas flow rate (e.g.,2 L/min) can also generate a larger effective plasma reaction zone with a longer arc length for chemical reactions.Two different motion patterns can be clearly observed in the N2 and air RGA plasmas.The time-resolved arc voltage signals show that three different arc dynamic modes,the arc restrike mode,takeover mode,and combined modes,can be clearly identified in the RGA plasmas.The occurrence of different motion and arc dynamic modes is strongly dependent on the composition of the working gas and gas flow rate.     

Investigation of optimum discharge characteristics and chemical activity of AC driven air plasma jet and its anticancer effect

In this study,we investigated the effects of the quartz tube diameter,air flow rate,and applied voltage on the characteristics of an air plasma jet to obtain the optimized discharge characteristics.The physicochemical properties and concentration of reactive oxygen and nitrogen species(RONS)in plasma-activated medium(PAM)were characterized to explore their chemical activity.Furthermore,we investigated the inactivation effect of air plasma jet on tumour cells and their corresponding inactivation mechanism.The results show that the tube diameter plays an important role in sustaining the voltage of the air plasma jet,and the gas flow rate affects the jet length and discharge intensity.Additionally,the air plasma jet discharge displays two modes,namely,ozone and nitrogen oxide modes at high and low gas flow rates,respectively.Increasing the voltage increases the concentration of reactive species and the length of discharge.By evaluating the viability of A549 cells under different parameters,the optimal treatment conditions were determined to be a quartz tube diameter of 4 mm,gas flow rate of 0.5 SLM,and voltage of 18 kV.Furthermore,an air plasma jet under the optimized conditions effectively enhanced the chemical activity in PAM and produced more aqueous RONS.The air plasma jet induced significant cytotoxicity in A549 cancer cells after plasma treatment.H2O2 and NO2 are regarded as key factors in promoting cell inactivation.The present study demonstrates the potential use of tumour cell therapy by atmospheric air PAM,which aids a better understanding of plasma liquid chemistry.     

Effects of Oxygen Concentration on Pulsed Dielectric Barrier Discharge in Helium-Oxygen Mixture at Atmospheric Pressure

In this work the effects of O_2 concentration on the pulsed dielectric barrier discharge in helium-oxygen mixture at atmospheric pressure have been numerically researched by using a one-dimensional fluid model in conjunction with the chosen key species and chemical reactions.The reliability of the used model has been examined by comparing the calculated discharge current with the reported experiments. The present work presents the following significant results. The dominative positive and negative particles are He_2~+ and O_2~-, respectively, the densities of the reactive oxygen species(ROS) get their maxima nearly at the central position of the gap, and the density of the ground state O is highest in the ROS. The increase of O_2 concentration results in increasingly weak discharge and the time lag of the ignition. For O_2 concentrations below 1.1%,the density of O is much higher than other species, the averaged dissipated power density presents an evident increase for small O_2 concentration and then the increase becomes weak. In particular,the total density of the reactive oxygen species reaches its maximums at the O_2 concentration of about 0.5%. This characteristic further convinces the experimental observation that the O_2 concentration of 0.5% is an optimal O_2/He ratio in the inactivation of bacteria and biomolecules when radiated by using the plasmas produced in a helium oxygen mixture.     

Numerical investigation of Ar–NH_3 mixture in homogenous DBDs

In this paper, a study of homogenous dielectric barrier discharge Ar–NH_3 was made in order to investigate the electrical and the physical characteristics of homogenous discharge at atmospheric pressure. The discharge model includes the electrical module and the chemical kinetic module. The results obtained by the present model were compared with experimental work. The evolution of the plasmas voltage, the species densities, and the concentration of charged species are analyzed and discussed.     

Thermodynamic and Transport Properties of Real Air Plasma in Wide Range of Temperature and Pressure

Air plasma has been widely applied in industrial manufacture. In this paper, both dry and humid air plasmas' thermodynamic and transport properties are calculated in temperature300–100000 K and pressure 0.1–100 atm. To build a more precise model of real air plasma, over 70 species are considered for composition. Two different methods, the Gibbs free energy minimization method and the mass action law method, are used to determinate the composition of the air plasma in a different temperature range. For the transport coefficients, the simplified Chapman-Enskog method developed by Devoto has been applied using the most recent collision integrals. It is found that the presence of CO_2 has almost no effect on the properties of air plasma. The influence of H_2O can be ignored except in low pressure air plasma, in which the saturated vapor pressure is relatively high. The results will serve as credible inputs for computational simulation of air plasma.     

Pattern Formation in a Dusty Plasma System

A rich variety of dust patterns have been observed in a capacitively coupled rf discharge dusty plasma system. Dust particles are synthesized through chemical reaction of the filled gas mixture during discharge. Different patterns are formed in different stages of particle growth. In the early stage of particle growth, dust cloud can be formed by a large number of small particles, and its behavior appears to be fluid-like. Such interesting nonlinear phenomena as dust void and complex dust cloud patterns are observed in this stage. As dust particles grow, the particle size and structure can be controlled to follow two different routes. In one of the routes, the particles grow up in a ball-like shape and can be formed into regular lattice and cluster patterns. In the other, the particles grow up in a fractal shape.     

Particle-in-cell/Monte Carlo simulation of filamentary barrier discharges

The plasma behavior of filamentary barrier discharges in helium is simulated using a twodimensional (2D) particle-in-cell/Monte Carlo model.Four different phases have been suggested in terms of the development of the discharge:the Townsend phase;the space-charge dominated phase;the formation of the cathode layer,and the extinguishing phase.The spatialtemporal evolution of the particle densities,velocities of the charged particles,electric fields,and surface charges has been demonstrated.Our simulation provides insights into the underlying mechanism of the discharge and explains many dynamical behaviors of dielectric barrier discharge (DBD) filaments.     

Influence of Ti3C2Tx(MXene)on the generation of dielectric barrier discharge in air

The formation of homogeneous dielectric barrier discharge(DBD)in air is a key scientific problem and core technical problem to be solved for the application of plasmas.Here,we report the effect of two-dimensional(2D)nanomaterial Ti3C2Tx(Tx=-F,-O and/or-OH)on regulating the electrical discharge characteristics.The field emission and weak bound state property of Ti3C2Tx can effectively increase the seed electrons and contribute to the generation of atmospheric pressure homogeneous air DBD.The electron avalanche development for the uneven electrode structure is calculated,and the discharge mode transition is modeled.The comparative analyses of discharge phenomena validate the regulation of Ti3C2Tx on the discharge characteristics of DBD.The light emission capture and the voltage and current waveforms verify that the transition of Townsend discharge to streamer discharge is effectively inhibited.The optical emission spectra are used to characterize the plasma and confirm that it is in a non-equilibrium state and the gas temperature is at room temperature.This is the first exploration of Ti3C2Tx on the regulation of electrical discharge characteristics as far as we know.This work proves the feasibility of Ti3C2Tx as a source of seed electrons to form homogeneous DBD,establishing a preliminary foundation for promoting the application of atmospheric pressure non-equilibrium plasma.     

A two-dimensional air streamer discharge modified model based on artificial stability term under non-uniform electric field at low temperature and sub-atmospheric pressure

In this paper, an improved air discharge fluid model under non-uniform electric field is constructed based on the plasma module COMSOL Multiphysics with artificial stability term, and the boundary conditions developed in the previous paper are applied to the calculation of photoionization rate. Based on the modified model, the characteristics of low temperature subatmospheric air discharge under 13 kV direct current voltage are discussed, including needle-plate and needle-needle electrode structures. Firstly, in order to verify the reliability of the model, a numerical example and an experimental verification were carried out for the modified model respectively. Both verification results show that the model can ensure the accuracy and repeatability of the calculation. Secondly, according to the calculation results of the modified model, under the same voltage and spacing, the reduced electric field under low temperature subatmosphere pressure is larger than that under normal temperature and atmospheric pressure. The high electric field leads to the air discharge at low temperature and sub atmospheric pressure entering the streamer initiation stage earlier, and has a faster propagation speed in the streamer development stage, which shortens the overall discharge time. Finally, the discharge characteristics of the two electrode structures are compared, and it is found that the biggest difference between them is that there is a pre-ionization region near the cathode in the needle-needle electrode structure. When the pre-ionization level reaches 10~(13) cm~(-3), the propagation speed of the positive streamer remains unchanged throughout the discharge process, and is no longer affected by the negative streamer. The peak value of electric field decreases with the increase of pre-ionization level, and tends to be constant during streamer propagation. Based on the previous paper, this paper constructs the air discharge model under non-uniform electric field, complements with the previous paper, and forms a relatively complete set of air discharge simulation system under low temperature and sub atmospheric pressure, which provides a certain reference for future research.     

The Role of Metastable Atoms in a Homogeneous Atmospheric Pressure Barrier Discharge in Helium

A one-dimensional fluid model for homogeneous atmospheric pressure barrier discharges in helium is presented by considering elementary processes of excitation and ionization including a metastable atom effect. Using this model we investigate the behaviours of the helium metastable atoms in discharges as well as their influence on the discharge characteristics. It is shown that the metastable atoms with a relatively high concentration during the discharge are mainly produced in the active phase of the discharge and dissolved in the off phase. It is also found that the metastable atom collisions can not only provide seed electrons for discharges but also influence the concentration of ions. A reduction of matestable atom density results in a drop in the charged particle densities and causes a qualitative change in the discharge patterns.     

Collision effects on propagation characteristics of electromagnetic waves in a sub-wavelength plasma slab of partially ionized dense plasmas

Intensive collisions between electrons and neutral particles in partially ionized plasmas generated in atmospheric/sub-atmospheric pressure environments can sufficiently affect the propagation characteristics of electromagnetic waves,particularly in the sub-wavelength regime.To investigate the collisional effect in such plasmas,we introduce a simplified plasma slab model with a thickness on the order of the wavelength of the incident electromagnetic wave.The scattering matrix method (SMM) is applied to solve the wave equation in the plasma slab with significant nonuniformity.Results show that the collisions between the electrons and the neutral particles,as well as the incident angle and the plasma thickness,can disturb the transmission and reduce reflection significantly.     

A comparative study on the activity of TiO2 in pulsed plasma under different discharge conditions

In the present study,a combination of pulsed discharge plasma and TiO_2(plasma/TiO_2)has been developed in order to study the activity of TiO_2by varying the discharge conditions of pulsed voltage,discharge mode,air flow rate and solution conductivity.Phenol was used as the chemical probe to characterize the activity of TiO_2in a pulsed discharge system.The experimental results showed that the phenol removal efficiency could be improved by about 10%by increasing the applied voltage.The phenol removal efficiency for three discharge modes in the plasma-discharge-alone system was found to be highest in the spark mode,followed by the spark–streamer mode and finally the streamer mode.In the plasma/TiO_2system,the highest catalytic effect of TiO_2was observed in the spark–streamer discharge mode,which may be attributed to the favorable chemical and physical effects from the spark–streamer discharge mode,such as ultraviolet light,O_3,H_2O_2,pyrolysis,shockwaves and high-energy electrons.Meanwhile,the optimal flow rate and conductivity were 0.05 m~3l~(-1)and 10μS cm~(-1),respectively.The main phenolic intermediates were hydroquinone,catechol,and p-benzoquinone during the discharge treatment process.A different phenol degradation pathway was observed in the plasma/TiO_2system as compared to plasma alone.Analysis of the reaction intermediates demonstrated that p-benzoquinone reduction was selectively catalyzed on the TiO_2surface.The effective decomposition of phenol constant(D_e)increased from 74.11%to 79.16%when TiO_2was added,indicating that higher phenol mineralization was achieved in the plasma/TiO_2system.     

Study of ionic wind based on dielectric barrier discharge of carbon fiber spiral electrode

Based on the idea that a large number of charged particles can be generated by a high-frequency alternating current(AC)dielectric barrier discharge(DBD),and charged particles can be accelerated directionally by a direct current(DC)electric field,a new type of ionic wind formation method is proposed in this paper.To this end,a carbon fiber spiral electrode serves as the generation electrode and a metal rod electrode as the collection electrode,with AC and DC potentials applied respectively to the generation electrode and the collection electrode to form an AC-DC coupled electric field.Under the action of the coupled electric field,a dielectric barrier discharge is formed on the carbon fiber spiral electrode,and the electrons generated by the discharge move from the generation electrode to the collection electrode in the opposite direction of the electric field vectors.During the movement,energy is transferred to the gas molecules by their colliding with neutral gas molecules,thereby forming a directional gas stream movement,i.e.ionic wind.In the research process,it is verified through electric field simulation analysis and discharge experiment that this method can effectively increase the number of charged particles in the discharge process,and the velocity of the ionic wind is nearly doubled.On this basis,the addition of a third electrode forms a distinct discharge region and an electron acceleration region,which further increases its velocity.The experimental result shows that the ionic wind speed reaches up to 2.98 m s^?1.Thanks to the ability of the electrode structure to generate an atmospheric pressure DBD plasma and form an ionic wind,we can create a noise-free air purification device without resorting to a fan,with this device having good application prospects in the field of air purification.     

Particle Densities of the Atmospheric-Pressure Argon Plasmas Generated by the Pulsed Dielectric Barrier Discharges

Atmospheric-pressure argon plasmas have received increasing attention due to their high potential in many industrial and biomedical applications. In this paper, a 1-D fluid model is used for studying the particle density characteristics of the argon plasmas generated by the pulsed dielectric barrier discharges. The temporal evolutions of the axial particle density distributions are illustrated, and the influences of changing the main discharge conditions on the averaged particle densities are researched by independently varying the various discharge conditions. The calculation results show that the electron density and the ion density reach two peaks near the momentary cathodes during the rising and the falling edges of the pulsed voltage. Compared with the charged particle densities, the densities of the resonance state atom Ar~r and the metastable state atom Ar~mhave more uniform axial distributions, reach higher maximums and decay more slowly. During the platform of the pulsed voltage and the time interval between the pulses, the densities of the excited state atom Ar*are far lower than those of the Ar~r or the Ar~m. The averaged particle densities of the different considered particles increase with the increases of the amplitude and the frequency of the pulsed voltage. Narrowing the discharge gap and increasing the relative dielectric constant of the dielectric also contribute to the increase of the averaged particle densities. The effects of reducing the discharge gap distance on the neutral particle densities are more significant than the influences on the charged particle densities.     

Exploration to generate atmospheric pressure glow discharge plasma in air

Atmospheric pressure glow discharge (APGD) plasma in air has high application value.In this paper,the methods of generating APGD plasma in air are discussed,and the characteristics of dielectric barrier discharge (DBD) in non-uniform electric field are studied.It makes sure that APGD in air is formed by DBD in alternating current electric field with using the absorbing electron capacity of electret materials to provide initial electrons and to end the discharge progress.Through designing electric field to form two-dimensional space varying electric field and three-dimensional space varying electric field,the development of electron avalanches in airgap is suppressed effectively and a large space of APGD plasma in air is generated.Further,through combining electrode structures,a large area of APGD plasma in air is generated.On the other hand,by using the method of increasing the density of initial electrons,millimeter-gap glow discharge in atmospheric pressure air is formed,and a maximum gap distance between electrodes is 8 ram.By using the APGD plasma surface treatment device composed of contact electrodes,the surface modification of high polymer materials such as aramid fiber and polyester are studied and good effect of modifications is obtained.The present paper provides references for the researchers of industrial applications of plasma.