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.     

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.     

Excited Electron Temperature and Molecular Vibration Temperature During Transition from Filamentary Discharge to Glow Discharge in Surface Discharge in Air

A dielectric barrier surface discharge device was used to investigate the transition from a filamentary discharge to a glow discharge in air at different gas pressures. Discharge images and waveforms of the applied voltage and discharge current were recorded simultaneously, and it was found that the discharge could transit from filamentary to glow with the decrease in pressure. Optical emission spectra during the transition from a filamentary discharge to a glow one were recorded. Excited electron temperature can be determined from the ratios of the relative intensities of spectral lines while molecular vibration temperature can be measured by analysing spectral lines of the N2 second positive band system. The results show that both the excited temperature and molecular vibration temperature increase with the decrease in the gas pressure. Qualitative explanations are given.     

Time-resolved measurements of NO2 concentration in pulsed discharges by high-sensitivity cavity ring-down spectroscopy

To describe the complex kinetics of formation and destruction mechanism of nitrogen dioxide(NO_2), there is an increasing demand for real-time and in situ analysis of NO_2 in the discharge region. Pulsed cavity ring-down spectroscopy(CRDS) provides an excellent diagnostic approach. In the present paper, CRDS has been applied in situ for time evolution measurement of NO_2 concentration which is rarely investigated in gas discharges. In pulsed direct current discharge of NO_2/Ar mixture at a pressure of 500 Pa, a peak voltage of -1300 V and a frequency of 30 Hz, for higher initial NO_2 concentration(3.05?×?10~(14)cm~(-3), 8.88?×?10~(13)cm~(-3)),the NO_2 concentration sharply decreases at the beginning of the discharge afterglow and then becomes almost constant, and the pace of decline increases with pulse duration; however, for lower initial NO_2 concentration of 1.69?×?10~(13)cm~(-3), the NO_2 concentration also decreases at the beginning of the discharge afterglow for 200 ns and 1 μs pulse durations, while it slightly increases and then declines for 2 μs pulse duration. Thus, the removal of low-level NO_2 could not be promoted by a higher mean energy input.     

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.     

Volume added surface barrier discharge plasma excited by bipolar nanosecond pulse power in atmospheric air: optical emission spectra influenced by gap distance

In this paper, volume barrier discharge with different gap distances is added on the discharge border of high-voltage electrode of annular surface barrier discharge for generating volume added surface barrier discharge (V-SBD) excited by bipolar nanosecond high-voltage pulse power in atmospheric air. The excited V-SBDs consist of surface barrier discharge (d=0 mm) and volume added surface barrier discharges (d=2 mm and 3 mm). The optical emission spectra are recorded for calculating emission intensities of N₂ (C ³Ⅱ_u →B³Π_g ) and N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ ), and simulating rotational and vibrational temperatures. The influences of gap distance of V-SBD on emission intensity and plasma temperature are also investigated and analyzed. The results show that d=0 mm structure can excite the largest emission intensity of N ₂ (C ³ Π_u →B ³Π_g ), while the existence of volume barrier discharge can delay the occurrence of the peak value of the emission intensity ratio of N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ )/N ₂(C³Π_u →B³Π_g ) during the rising period of the applied voltage pulse and weaken it during the end period. The increasing factor of emission intensity is effected by the pulse repetition rate. The d=3 mm structure has the highest threshold voltage while it can maintain more emission intensity of N₂(C³ Π _u →B ³Π_g ) than that of d=2 mm structure. The structure of d=2 mm can maintain more increasing factor than that of the d=3 mm structure with varying pulse repetition rate. Besides, the rotational temperatures of three V-SBD structures are slightly affected when the gap distance and pulse repetition rate vary. The vibrational temperatures have decaying tendencies of all three structures with the increasing pulse repetition rate.     

Atmospheric air dielectric barrier discharge excited by nanosecond pulse and AC used for improving the hydrophilicity of aramid fibers

In this paper, a long line-shape dielectric barrier discharge excited by a nanosecond pulse and AC is generated in atmospheric air for the purpose of discussing the uniformity, stability and ability of aramid fiber treatment. The discharge images, waveforms of current and voltage,optical emission spectra, and gas temperatures of both discharges are compared. It is found that nanosecond pulsed discharge has a more uniform discharge morphology, higher energy efficiency and lower gas temperature, which indicates that nanosecond pulsed discharge is more suitable for surface modification. To reduce the water contact angle from 96° to about 60°, the energy cost is only about 1/7 compared with AC discharge. Scanning electron microscopy,Fourier transform infrared spectroscopy and x-ray photoelectron spectroscopy are employed to understand the mechanisms of hydrophilicity improvement.     

Influence of the Gas Mixture Ratio on the Correlations Between the Excimer XeCl Emission and the Sealed Gas Temperature in DIelectric Barrier Discharge Lamps

For dielectric barrier discharge lamps filled with various gas mixture ratios,the correlations between the excimer XeCl emission and the sealed gas temperature have been founded,and a qualitative explication is presented.For gas mixture with chlorine larger than 3%,the emission intensity increases with the sealed gas temperature,while with chlorine about 2%,the emission intensity decreases with the increase in the gas temperature,and could be improved by cooling water .However,if chlorine is less than 1.5% ,the discharge appears to be a mixture mode with filaments distributed in a diffused glow-like discharge,and the UV emission is independent on the gas temperature.     

Experiment and Analysis on the Treatment of Gaseous Benzene Using Pulsed Corona Discharge Plasma

An experiment and analysis on removal of gaseous benzene by pulse corona inducedplasma is presented in this article. Important parameters effecting removal efficiency have been investigated, such as pulse peak voltage, pulse frequency, gas inlet concentration, gas flow rate and reactor temperature. The result shows that the removal efficiency increases with the increase in pulse peak voltage, pulse frequency and reactor temperature, but decreases in the rise of gas inlet concentration and gas flow rate. On the condition of Vp = 36 kV, f = 80 Hz, C = 1440 mg/m^3 and Q = 640 ml/min, the largest removal efficiency is 98%. Finally, the reacted products are qualitatively analysed and the reaction processes are deduced in combination with plasma-chemistry theory.     

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.     

Atmospheric Pressure Radio Frequency Dielectric Barrier Discharges in Nitrogen/Argon

This work reports the experimental results on the characteristics of radio frequency dielectric barrier N2 /Ar discharges.Depending on the nitrogen content in the feed gas and the input power,the discharge can operate in two diferent modes: a homogeneous glow discharge and a constricted discharge.With increasing input power,the number of discharge columns increases.The discharge columns have starlike structures and exhibit symmetric self-organized arrangement.Optical emission spectroscopy was performed to estimate the plasma temperature.Spatially resolved gas temperature measurements,determined from NO emission rotational spectroscopy were taken across the 4.4 mm gap filled by the discharge.Gas temperature in the middle of the gas gap is lower than that close to the electrodes.     

Temporal evolution of atmospheric cascade glow discharge with pulsed discharge and radio frequency discharge

Atmospheric cascade discharges with pulsed discharge and radio frequency(RF)discharge were experimentally investigated by the temporal evolution of discharge spatial profile and intensity.The indium tin oxide(ITO)coated glass was employed as the transparent electrode to capture the discharge distribution above the electrode surface.It is demonstrated that in the pulsed discharge with dielectric barrier,the first discharge at the rising edge of pulse voltage is uniformly ignited and then forms an expanding plasma ring on the ITO electrode surface,which shrinks to the same diameter as that of bare stainless steel electrode with the generation of second discharge at the falling edge of pulse voltage.The discharge profiles along the electrode surface and discharge gap of the successive RF discharge are dependent on the intensity and spatial distribution of residual plasma species generated by the pulsed discharge,which is determined by the time interval between the pulsed discharge and RF discharge.It is demonstrated that the residual plasma species before the RF discharge ignition help to achieve the stable operation of RF discharge with elevated intensity.     

Effect of Airflows on Repetitive Nanosecond Volume Discharges

Atmospheric pressure discharges excited by repetitive nanosecond pulses have attracted significant attention for various applications.In this paper,a plate-plate discharge with airflows is excited by a repetitive nanosecond pulse generator.Under different experiment conditions,the applied voltages,discharge currents,and discharge images are recorded.The plasma images presented here indicate that the volume discharge modes vary with airflow speeds,and a diffuse and homogeneous volume discharge occurs at the speed of more than 35 m/s.The role of airflows provides different effects on the 2-stage pulse discharges.The 1st pulse currents nearly maintain consistency for different airflow speeds.However,the 2nd pulse current has a change trend of first decreasing and then rapidly increasing,and the value difference for 2nd pulse currents is about 20 A under different airflows.In addition,the experimental results are discussed according to the electrical parameters and discharge images.     

Parametric study of high-frequency characteristics of plasma synthetic jet actuator

A major issue of plasma synthetic jet actuator(PSJA)is the severe performance deterioration at high working frequency.In this study,experiments and numerical simulation are combined together to investigate the influence of thermal conductivity,throat length(Lth)and discharge duration(Td)on the high-frequency characteristics of PSJA.Results show that the variation of the actuator thermal conductivity and discharge duration will not alter the saturation frequency of the actuator,whereas decreasing the throat length results in an increase of the saturation frequency.For a short-duration capacitive discharge of 1.7 μs,a clear shock wave is issued from the orifice,followed by a weak jet.As a comparison,when the discharge duration is increased up to 202.6 μs,a strong jet column is formed and no obvious shock wave can be visualized.Based on numerical simulation results,it becomes clear that the long-duration pulse-DC discharge is able to heat the cavity gas to a much higher temperature(3141K)than capacitive discharge,greatly improving the conversion efficiency of the arc discharge energy to the internal energy of the cavity gas.In addition,high-speed Schlieren imaging is deployed to study the performance degradation mechanism of PSJA at high working frequency.Monitor of the exit jet grayscale indicates that as long as the saturation frequency is exceeded,the actuator becomes unstable due to insufficient refresh time.The higher the discharge frequency,the more frequently the phenomenon of'misfires'will occur,which explains well the decaying jet total pressure at above saturation frequency.     

Evaluation on a double-chamber gas-liquid phase discharge reactor for benzene degradation

A double-chamber gas-liquid phase DBD reactor (GLDR), consisting of a gas-phase discharge chamber and a gas-liquid discharge chamber in series, was designed to enhance the degradation of benzene and the emission of NOx. The performance of the GLDR on discharge characteristics, reactive species production and benzene degradation was compared to that of the single-chamber gas phase DBD reactor (GPDR). The effects of discharge gap, applied voltage, initial benzene concentration, gas flow rate and solution conductivity on the degradation and energy yield of benzene in the GLDR were investigated. The GLDR presents a higher discharge power, higher benzene degradation and higher energy yield than that of the GPDR. NO₂ emission was remarkably inhibited in the GLDR, possibly due to the dissolution of NO₂ in water. The benzene degradation efficiency increased with the applied voltage, but decreased with the initial concentration, gas flow rate, and gas discharge gap, while the solution conductivity presented less influence on benzene degradation. The benzene degradation efficiency and the energy yield reached 61.11% and 1.45 g kWh^–1 at 4 mm total gas discharge gap, 15 kV applied voltage, 200 ppm benzene concentration, 0.2 L min⁻¹ gas flow rate and 721 μS cm⁻¹ water conductivity. The intermediates and byproducts during benzene degradation were detected by FT-IR, GC-MS and LC-MS primarily, and phenols, CO_x, and other aromatic substitutes, O₃, NO_x, etc, were determined as the main intermediates. According to these detected byproducts, a possible benzene degradation mechanism was proposed.     

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.     

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.     

Experimental study on the parameter optimization and application of a packed-bed dielectric barrier discharge reactor in diesel particulate filter regeneration

To compensate for the shortcomings of the thermal and catalytic regeneration of the diesel particulate filter(DPF),a self-designed packed-bed dielectric barrier discharge(DBD)reactor for DPF regeneration was developed.The DBD reactor with the main active substance of nonthermal plasma(NTP)as the target parameter was optimized by adjusting the feed gas,packing particles(material or size),and cooling water temperature.Moreover,a set of optimal working parameters(gas source,O2;packing particles,1.2-1.4 mm ZrO2;and cooling water temperature,20℃)was selected to evaluate the effect of different O3 concentrations on DPF regeneration.The research results showed that selecting packing particles with high dielectric constant and large particles,as well as reducing the cooling water temperature,with oxygen as the feed gas,contributed to an increase in O3 concentration.During DPF regeneration,the following changes were observed:the power of the NTP reactor decreased to lower than 100 W,the O3 concentration increased from 15 g m-3 to 45 g m-3,the CO and CO2 volume fractions of the particulate matter decomposition products increased,and the peak regeneration temperature increased to 173.4℃.The peak temperature arrival time was 60 min earlier,indicating that the regeneration rate of DPF increased with the increase in O3 concentration.However,the O3 utilization rate(the amount of carbon deposit removed per unit volume O3)initially increased and then decreased;when the O3 concentration was set to 25 g m-3,the highest O3 utilization rate was reached.The packed-bed DBD technology contributed to the increase in the concentration of NTP active substances and the regeneration efficiency of DPF.It provides a theoretical and experimental basis for high-efficiency regeneration of DPF at low temperatures(＜200℃).     

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.     

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.