Generation of reactive atomic species of positive pulsed corona discharges in wetted atmospheric flows of nitrogen and oxygen

The emission spectra of excited radicals(OH(A~2E),O(3p~3 P),H_α(3P)) and emissive species(N_2~+(B~2∑_u~+),N_2(C_3Π_u)) produced by positive pulsed high-voltage needle-plane corona discharges in atmospheric N_2 and O_2 flows wetted with 10%H_2O at 80 ℃ are used to investigate the relative concentrations of the produced radicals.The results indicate that the tendencies of the concentrations of radicals with discharge conditions are similar to each other due to their similar excitation processes by electron collision.The influence of oxygen flow mixed with the nitrogen flow on the emission intensities of O(3p~5P → 3s~5S_2~.),H_α(3P → 2S),N_2_+(B~2∑_u~+ → X~2∑_g+0-0),and N_2(C~3Π_u → B~3Π_g 1-0) is presented.When the flow rate of oxygen addition is varied from 0-30 ml min~(-1),the emission intensities of O(3p~5P → 3s~5S_2~0.),H_α(3P → 2s),and N_2~+(B~2∑_u~+ →X~2∑_g 0-0) increase and reach a maximum.Then,if the oxygen flow rate increases further,the emission intensities tend to decrease.However,the intensity of N_2(C~3Π_u → B~3Π_g1-0) decreases monotonously with the increasing oxygen flow,which indicates that the electron density decreases with the increasing oxygen flow.By the tendencies of the relative intensities to N_2(C~3Π_u → B~3Π_g 1-0),the concentrations of the total produced O,H,and N_2~+ are shown to increase with the oxygen flow.Based on the reactions for the production of H and O without and with the addition of O_2,the analytic solutions for H and O production are derived in accordance with the experimental results.     

Measurement of the first Townsend's ionization coefficient for atmospheric pressure neon by a dielectric barrier discharge

Fast photography and optical emission spectroscopy are implemented in a 5 mm neon gap dielectric barrier discharge (DBD) at atmospheric pressure with quartz glass used as the dielectric layer. Results show that it starts with a Townsend discharge and ends at a sub-normal glow discharge in neon DBD. Based on the Townsend discharge, the first ionization coefficient of neon is measured. The measurements are consistent with those at low pressure. Optical emission spectroscopy indicates that the spectra are mainly composed of atomic lines of neon, molecular bands and molecular ion bands originating from inevitable gas impurities (mainly nitrogen). Moreover, spectral lines emitted from atomic neon corresponding to the transitions (2p⁵ 3p → 2p⁵ 3s) are predominant. Although the second positive system of N₂(C³Π_u → B³Π_g) is observed, their intensities are too weak compared with neon's spectrum. The molecular nitrogen ion line of 391.4 nm is observed. It reveals that Penning ionization between high energy neon excited states and the inevitable gas impurities plays an important role in the value of the α coefficient.     

Electrical characters and optical emission spectra of VBD coupled SBD excited by sine AC voltage in atmospheric air

In this paper,volume coupled surface barrier discharge(V-SBD) with three structures possessing different volumes is excited by sine AC power in atmospheric air.Discharge images,waveforms of applied voltage and discharge current,and optical emission spectra simulating rotational and vibrational temperatures are recorded and analyzed.The effects of applied voltage on emission intensities of N_2(C~3Π_u→ B~3Π_g) and N_2~+(B~2∑_u~+ → X~2E_g~+),and rotational and vibrational temperatures are investigated.The results show that as applied voltage rises,emission intensities and rotational temperatures increase while vibrational temperatures decrease.In addition it is found that,as applied voltage varies,the rotational temperature of surface discharge changes faster than that of volume discharge.     

Discharge Modes Suggested by Emission Spectra of Nitrogen Dielectric Barrier Discharge with Wire-Cylinder Electrodes

In this paper,nitrogen dielectric barrier discharge(DBD) plasma was generated in a quartz tube with coaxial wire-cylinder electrodes at atmospheric pressure.By varying the nitrogen gas flow(FN) in the range of 0-1 m3/h,the plasma optical emission spectra(OES) were measured and studied.The vibration(T_(vib)) and rotation temperature(T_(rot)) of nitrogen were obtained,by fitting the rovibronic bands of N_2(C~3∏_u-B~3∏_g,0-1),and by the Boltzmann plot method for purposes of comparison.T_(vib) increased up to 2481 K with increasing nitrogen flow till0.2 m3/h,and then decreased with further increasing FN,while Trot decreased monotonously and approached to-350 K for FN ≥ 0.6 m~3/h.The intensity of N_2(C~3∏_u-B~3∏_g,0-0,1-0,0-3) and N_2~+(B~2∑_u~+-X~2Σ_g~+,0-0) exhibited similar evolution with increasing FN to those of the T_(vib) and Trot,respectively.The discharge photos revealed that the discharge filaments gradually decreased with increasing FN,and eventually disappeared,which implied that a discharge mode transition emerged with increasing FN.The possible mechanism for the discharge mode transition is studied in detail according to the vibration(T_(vib)) and rotation temperature(T_(rot)) of nitrogen.     

Discharge characteristics and reactive species production of unipolar and bipolar nanosecond pulsed gas-liquid discharge generated in atmospheric

In this paper,unipolar pulse (including positive pulse and negative pulse) and bipolar pulse voltage are employed to generate diffuse gas-liquid discharge in atmospheric N2 with a trumpet-shaped quartz tube.The current-voltage waveforms,optical emission spectra of excited state active species,FTIR spectra of exhaust gas components,plasma gas temperature,and aqueous H2O2,NO2-,and NO3-production are compared in three pulse modes,meanwhile,the effects of pulse peak voltage and gas flow rate on the production of reactive species are studied.The results show that two obvious discharges occur in each voltage pulse in unipolar pulse driven discharge,differently,in bipolar pulse driven discharge,only one main discharge appears in a single voltage pulse time.The intensities of active species (OH(A),and O(3p)) in all three pulsed discharge increase with the rise of pulse peak voltage and have the highest value at 200 ml min-1 of gas flow rate.The absorbance intensities of NO2 and N2O increase with the increase of pulse peak voltage and decrease with the increase of gas flow rate.Under the same discharge conditions,the bipolar pulse driven discharge shows lower breakdown voltage,and higher intensities of excited species (N2(C),OH(A),and O(3p)),nitrogen oxides (NO2,NO,and N2O),and higher production of aqueous H2O2,NO2-,and NO3-compared with both unipolar positive and negative discharges.     

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.     

Spectroscopic study of bipolar nanosecond pulse gas-liquid discharge in atmospheric argon

Atmospheric gas-liquid discharge with argon as a working gas is presented by employed nanosecond pulse power. The discharge is presented in a glow-like mode. The discharge powers are determined to be less than 1 W, and remains almost constant when the discharge duration time increases. Bountiful active species are determined by capturing optical emission spectra,and their main generation processes are also discussed. The plasma gas temperature is calculated as 350 K by comparing the experimental spectra and the simulated ones of N_2(C~3Ⅱ_g→B~3Ⅱ_g, Δv =-2). The time resolved vibrational and rotational temperature is researched to present the stability of discharge when pulse voltage and discharge duration vary.The electron density is determined to be 10~(16) cm~(-3) according to the Stark broadening effect of the H_α line.     

Discharge characteristics and reactive species production of unipolar and bipolar nanosecond pulsed gas–liquid discharge generated in atmospheric N_2

In this paper,unipolar pulse (including positive pulse and negative pulse) and bipolar pulse voltage are employed to generate diffuse gas–liquid discharge in atmospheric N_2with a rumpetshaped quartz tube.The current–voltage waveforms,optical emission spectra of excited state active species,FTIR spectra of exhaust gas components,plasma gas temperature,and aqueous H_2O_2,NO_2~-,andNO_3~-production are compared in three pulse modes,meanwhile,the effects of pulse peak voltage and gas flow rate on the production of reactive species are studied.The results show that two obvious discharges occur in each voltage pulse in unipolar pulse driven discharge,differently,in bipolar pulse driven discharge,only one main discharge appears in a single voltage pulse time.The intensities of active species (OH(A),and O(3p)) in all three pulsed discharge increase with the rise of pulse peak voltage and have the highest value at 200 ml min~(-1)of gas flow rate.The absorbance intensities of NO_2and N_2O increase with the increase of pulse peak voltage and decrease with the increase of gas flow rate.Under the same discharge conditions,the bipolar pulse driven discharge shows lower breakdown voltage,and higher intensities of excited species (N_2(C),OH(A),and O(3p)),nitrogen oxides (NO_2,NO,and N_2O),and higher production of aqueous H_2O_2,NO_2~-,andNO_3~-compared with both unipolar positive and negative discharges.     

Effects of O2 addition on the plasma uniformity and reactivity of Ar DBD excited by ns pulsed and AC power supplies

Dielectric barrier discharges (DBDs) have been widely used in ozone synthesis, materials surface treatment, and plasma medicine for their advantages of uniform discharge and high plasma-chemical reactivity. To improve the reactivity of DBDs, in this work, the O₂ is added into Ar nanosecond (ns) pulsed and AC DBDs. The uniformity and discharge characteristics of Ar ns pulsed and AC DBDs with different O₂ contents are investigated with optical and electrical diagnosis methods. The DBD uniformity is quantitatively analyzed by gray value standard deviation method. The electrical parameters are extracted from voltage and current waveforms separation to characterize the discharge processes and calculate electron density n_e. The optical emission spectroscopy is measured to show the plasma reactivity and calculate the trend of electron temperature T_e with the ratio of two emission lines. It is found that the ns pulsed DBD has a much better uniformity than AC DBD for the fast rising and falling time. With the addition of O₂, the uniformity of ns pulsed DBD gets worse for the space electric field distortion by O₂⁻, which promotes the filamentary formation. While, in AC DBD, the added O₂ can reduce the intensity of filaments, which enhances the discharge uniformity. The ns pulsed DBD has a much higher instantaneous power and energy efficiency than AC DBD. The ratio of Ar emission intensities indicates that the T_e drops quickly with the addition of O₂ both ns pulsed and AC DBDs and the ns pulsed DBD has an obvious higher T_e and n_e than AC DBD. The results are helpful for the realization of the reactive and uniform low temperature plasma sources.     

OH and O radicals production in atmospheric pressure air/Ar/H2O gliding arc discharge plasma jet

Atmospheric pressure air/Ar/H_2O gliding arc discharge plasma is produced by a pulsed dc power supply. An optical emission spectroscopic(OES) diagnostic technique is used for the characterization of plasmas and for identifications of OH and O radicals along with other species in the plasmas. The OES diagnostic technique reveals the excitation Tx?≈?5550–9000 K, rotational Tr?≈?1350–2700 K and gas Tg?≈?850–1600 K temperatures, and electron density n?(1.1-1.9) ′101 4 cm~(-3) e under different experimental conditions. The production and destruction of OH and O radicals are investigated as functions of applied voltage and air flow rate. Relative intensities of OH and O radicals indicate that their production rates are increased with increasing Ar content in the gas mixture and applied voltage. nereveals that the higher densities of OH and O radicals are produced in the discharge due to more effective electron impact dissociation of H_2O and O_2 molecules caused by higher kinetic energies as gained by electrons from the enhanced electric field as well as by enhanced n e.The productions of OH and O are decreasing with increasing air flow rate due to removal of Joule heat from the discharge region but enhanced air flow rate significantly modifies discharge maintenance properties. Besides, Tgsignificantly reduces with the enhanced air flow rate. This investigation reveals that Ar plays a significant role in the production of OH and O radicals.     

Investigation on discharge characteristics of a coaxial dielectric barrier discharge reactor driven by AC and ns power sources

A coaxial dielectric barrier discharge(DBD) reactor with double layer dielectric barriers has been developed for exhaust gas treatment and excited either by AC power or nanosecond(ns)pulse to generate atmospheric pressure plasma. The comparative study on the discharge characteristics of the discharge uniformity, power deposition, energy efficiency, and operation temperature between AC and ns pulsed coaxial DBD is carried out in terms of optical and electrical characteristics and operation temperature for optimizing the coaxial DBD reactor performance. The voltages across the air gap and dielectric layer and the conduction and displacement currents are extracted from the applied voltages and measured currents of AC and ns pulsed coaxial DBDs for the calculation of the power depositions and energy efficiencies through an equivalent electrical model. The discharge uniformity and operating temperature of the coaxial DBD reactor are monitored and analyzed by optical images and infrared camera. A heat conduction model is used to calculate the temperature of the internal quartz tube. It is found that the ns pulsed coaxial DBD has a much higher instantaneous power deposition in plasma, a lower total power consumption, and a higher energy efficiency compared with that excited by AC power and is more homogeneous and stable. The temperature of the outside wall of the AC and ns pulse excited coaxial DBD reaches 158 ℃ and 64.3 ℃ after 900 s operation, respectively.The experimental results on the comparison of the discharge characteristics of coaxial DBDs excited by different powers are significant for understanding of the mechanism of DBDs,reducing energy loss, and optimizing the performance of coaxial DBD in industrial applications.     

Generation of reactive species in atmospheric pressure dielectric barrier discharge with liquid water

Atmospheric pressure helium/water dielectric barrier discharge(DBD) plasma is used to investigate the generation of reactive species in a gas–liquid interface and in a liquid. The emission intensity of the reactive species is measured by optical emission spectroscopy(OES)with different discharge powers at the gas–liquid interface. Spectrophotometry is used to analyze the reactive species induced by the plasma in the liquid. The concentration of OH radicals reaches 2.2 μm after 3 min of discharge treatment. In addition, the concentration of primary longlived reactive species such as H_2O_2, NO_3~- and O_3 are measured based on plasma treatment time.After 5 min of discharge treatment, the concentration of H_2O_2, NO_3~-, and O_3 increased from 0 mg?·?L~(-1) to 96 mg?·?L~(-1), 19.5 mg?·?L~(-1), and 3.5 mg?·?L~(-1), respectively. The water treated by plasma still contained a considerable concentration of reactive species after 6 h of storage. The results will contribute to optimizing the DBD plasma system for biological decontamination.     

Influence of electrical parameters on H2O2 generation in DBD non-thermal reactor with water mist

A dielectric barrier discharge (DBD) reactor is introduced to generate H2O2 by non-thermal plasma with a mixture of oxygen and water mist produced by an ultrasonic atomizer.The results of our experiment show that the energy yield and concentration of the generated H2O2 in the pulsed discharge are much higher than that in AC discharge,due to its high energy efficiency and low heating effect.Micron-sized liquid droplets produced by an ultrasonic atomizer in water mist have large specific surface area,which greatly reduces mass transfer resistance between hydroxyl radicals and water liquids,leading to higher energy yield and H2O2 concentration than in our previous research.The influence of applied voltage,discharge frequency,and environmental temperature on the generated H2O2 is discussed in detail from the viewpoint of the DBD mechanism.The H2O2 concentration of 30 mg 1-1,with the energy yield of 2 g kW-1h 1 is obtained by pulsed discharge in our research.     

Degradation of Acid Orange 7 Dye in Two Hybrid Plasma Discharge Reactors

To get an optimized pulsed electrical plasma discharge reactor and to increase the energy utilization efficiency in the removal of pollutants, two hybrid plasma discharge reactors were designed and optimized. The reactors were compared via the discharge characteristics, energy transfer efficiency, the yields of the active species and the energy utilization in dye wastewater degradation. The results showed that under the same AC input power, the characteristics of the discharge waveform of the point-to-plate reactor were better. Under the same AC input power, the two reactors both had almost the same peak voltage of 22 kV. The peak current of the point-to-plate reactor was 146 A, while that of the wire-to-cylinder reactor was only 48.8 A. The peak powers of the point-to-plate reactor and the wire-to-cylinder reactor were 1.38 MW and 1.01 MW, respectively. The energy per pulse of the point-to-plate reactor was 0.2221 J, which was about 29.4% higher than that of the wire-to-cylinder reactor （0.1716 J）. To remove 50% Acid Orange 7 （AO7）, the energy utilizations of the point-to-plate reactor and the wire- to-cylinder reactor were 1.02×10^-9 mol/L and 0.61×10^-9 mol/L, respectively. In the point-to- plate reactor, the concentration of hydrogen peroxide in pure water was 3.6 mmol/L after 40 min of discharge, which was higher than that of the wire-to-cylinder reactor （2.5 mmol/L）. The concentration of liquid phase ozone in the point-to-plate reactor （5.7×10^-2 mmol/L） was about 26.7% higher than that in the wire-to-cylinder reactor （4.5×10^-2 mmol/L）. The analysis results of the variance showed that the type of reactor and reaction time had significant impacts on the yields of the hydrogen peroxide and ozone. The main degradation intermediates of AO7 identified by gas chromatography and mass spectrometry （GCMS） were acetic acid, maleic anhydride, p- benzoquinone, phenol, benzoic acid, phthalic anhydride, coumarin and 2-naphthol. Proposed degradation pathways were elucidated in light of the ana     

Spatiotemporal characteristics of nanosecond pulsed discharge in an extremely asymmetric electric field at atmospheric pressure

In this paper,high resolution temporal-spatial diagnostics are employed to research the optical characteristics of nanosecond pulsed dielectric barrier discharge in needle-plate electrode configuration.Temporal-spatial distributions of discharge images,the emission intensities of opticaI emission spectra,and plasma vibrational and rotational temperatures are investigated.By analyzing the evolution of vibrational and rotational temperatures in space and time dimensions,the energy distribution and energy transfer process in plasma are also discussed.It is found that a diffuse structure with high density plasma concentrated in the region near the needle tip can be presented in nanosecond pulsed discharge,and an obvious energy transfer from electronic energy to vibration energy can be observed in each discharge pulse.     

Plasma-Assisted Chemical Vapor Deposition of Titanium Oxide Films by Dielectric Barrier Discharge in TiCl_4/O_2/N_2 Gas Mixtures

Low-pressure dielectric barrier discharge（DBD） TiCl4/O2and N2 plasmas have been used to deposit titanium oxide films at different power supply driving frequencies. A homemade large area low pressure DBD reactor was applied, characterized by the simplicity of the experimental set-up and a low consumption of feed gas and electric power, as well as being easy to operate. Atomic force microscopy, scanning electron microscopy, energy dispersive spectroscopy,and contact angle measurements have been used to characterize the deposited films. Experimental results show all deposited films are uniform and hydrophilic with a contact angle of about 15 o.Compared to titanium oxide films deposited in TiCl4/O2gas mixtures, those in TiCl4/O2/N2gas mixtures are much more stable. The contact angle of titanium oxide films in TiCl4/O2/N2gas mixtures with the addition of 50% N2 and 20% TiCl4 is still smaller than 20 o, while that of undoped titanium oxide films is larger than 64 owhen they are measured after one week. The low-pressure TiCl4/O2plasmas consist of pulsed glow-like discharges with peak widths of several microseconds, which leads to the uniform deposition of titanium oxide films. Increasing a film thickness over several hundreds of nm leads to the film’s fragmentation due to the over-high film stress. Optical emission spectra（OES） of TiCl4/O2DBD plasmas at various power supply driving frequencies are presented.     

Characteristics of a kHz helium atmospheric pressure plasma jet interacting with two kinds of targets

This study investigates the influence of two types of target,skin tissue and cell culture medium,with different permittivities on a k Hz helium atmospheric pressure plasma jet (APPJ) during its application for wound healing.The basic optical–electrical characteristics,the initiation and propagation and the emission spectra of the He APPJ under different working conditions are explored.The experimental results show that,compared with a jet freely expanding in air,the diameter and intensity of the plasma plume outside the nozzle increase when it interacts with the pigskin and cell culture medium targets,and the mean velocity of the plasma bullet from the tube nozzle to a distance of 15 mm is also significantly increased.There are also multiple increases in the relative intensity of OH (A~2Σ?→?X~2Π) and O (3p~5S–3s~5S) at a position 15 mm away from nozzle when the He APPJ interacts with cell culture medium compared with the air and pigskin targets.Taking the surface charging of the low permittivity material capacitance and the strengthened electric field intensity into account,they make the various characteristics of He APPJ interacting with two different targets together.     

Plasma propagation in single-particle packed dielectric barrier discharges: joint effects of particle shape and discharge gap

In this work, a single Al₂O₃ particle packed dielectric barrier discharge (DBD) reactor with adjustable discharge gap is built, and the influences of the particle shape (ball and column) and the residual gap between the top electrode and particle on the electrical and optical characteristics of plasma are studied. Our research confirms that streamer discharge and surface discharge are the two main discharge patterns in the single-particle packed DBD reactor. The strong electric field distortion at the top of the ball or column caused by the dielectric polarization effect is an important reason for the formation of streamer discharge. The length of streamer discharge is proportional to the size of the residual gap, but the number of discharge times of a single voltage cycle shows an opposite trend. Compared to the column, a smooth spherical surface is more conducive to the formation of large and uniform surface discharges. The surface discharge area and the discharge intensity reach a maximum when the gap is equal to the diameter of the ball. All in all, the results of this study will provide important theoretical support for the establishment of the synergistic characteristics of discharge and catalysis in plasma catalysis.     

Performance of Dielectric Barrier Discharge Reactors on Elemental Mercury Oxidation in the Coal-Fired Flue Gas

The oxidation of elemental mercury （Hg~） by dielectric barrier discharge reactors was studied at room temperature, where concentric cylinder discharge reactor （CCDR） and surface discharge plasma reactor （SDPR） were employed. The parameters （e.g. Hg^0 oxidation efficiency, energy constant, energy yield, energy consumption, and O3 concentration） were discussed. From comparison of the two reactors, higher Hg^0 oxidation efficiency and energy constant in the SDPR system were obtained by using lower specific energy density. At the same applied voltage, energy yield in the SDPR system was larger than that in the CCDR system, and energy consumption in the SDPR system was much less. Additionally, more 03 was generated in the SDPR system. The experimental results showed that 98% of Hg^0 oxidation efficiency, 0.6 J·L^-1 of energy constant, 13.7 μg·J^-1 of energy yield, 15.1 eV·molecule^-1 of energy consumption, and 12.7 μg·J^-1 of O3 concentration were achieved in the SDPR system. The study reveals an alternative and economical technology for Hg^0 oxidation in the coal-fired flue gas.     

Conversion of NO with a catalytic packed-bed dielectric barrier discharge reactor

This paper discusses the conversion of nitric oxide (NO) with a low-temperature plasma induced by a catalytic packed-bed dielectric barrier discharge (DBD) reactor.Alumina oxide (Al2O3),glass (SiO2) and zirconium oxide (ZrO2),three different spherical packed materials of the same size,were each present in the DBD reactor.The NO conversion under varying input voltage and specific energy density,and the effects of catalysts (titanium dioxide (TiO2) and manganese oxide (MnOx) coated on Al2O3) on NO conversion were investigated.The experimental results showed that NO conversion was greatly enhanced in the presence of packed materials in the reactor,and the catalytic packed bed of MnOx/Al2O3 showed better performance than that of TiO2/Al2O3.The surface and crystal structures of the materials and catalysts were characterized through scanning electron microscopy analysis.The final products were clearly observed by a Fourier transform infrared spectrometer and provided a better understanding of NO conversion.