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.     

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.     

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.     

Degradation of Microcystin-LR by Gas-Liquid Interfacial Discharge Plasma

In this study, we report on the degradation of microcystin-LR （MC-LR） by gas- liquid interracial discharge plasma. The influences of operation parameters such as average input voltage, electrode distance and gas flow rate are investigated. Experimental results indicate that the input voltage and gas flow rate have positive influences on MC-LR degradation, while the electrode distance has a negative one. After 6 min discharge with 25 kV average input voltage and 60 L/h air aerati by discharge both in on, the degradation rate of MC-LR achieves 75.3%. distilled water and MC-LR solution are measured H202 and 03 generated Moreover, an emission spectroscopy is used as an indicator of the processes that take place on the gas-liquid boundary and inside plasma. Varied types of radicals （O, .OH, CO, 03, etc.） are proved to be present in the gas phase during gas-liquid interfacial discharge.     

Spectroscopic diagnosis of plasma in atmospheric pressure negative pulsed gasliquid discharge with nozzle-cylinder electrode

The plasma characteristics of a gas-liquid phase discharge reactor were investigated by optical and electrical methods.The nozzle-cylinder electrode in the discharge reactor was supplied witha negative nanosecond pulsed generator.The optical emission spectrum diagnosis revealed that OH(A~2∑~+?→?X~2Π,306–309 nm),N~3_2(CΠ→B~3Π_g,337 nm),O(3p~5p→3s~5s~0,777.2 nm)and O(3p~3p→3s~3s~0,844.6 nm)were produced in the discharge plasma channels.The electron temperature(T_e)was calculated from the emission relative intensity ratio between the atomic O 777.2 nm and 844.6 nm,and it increased with the applied voltage and the pulsed frequency and fell within the range of 0.5–0.8 e V.The gas temperature(T_g)that was measured by Lifbase was in a range from 400 K to 600 K.     

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.     

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.     

The investigation of OH radicals produced in a DC glow discharge by laser-induced fluorescence spectrometry

In this paper the OH radicals produced by a needle-plate negative DC discharge in water vapor,N2 + H2O mixture gas and He + H2O mixture gas are investigated by a laser-induced fluorescence (LIF) system.With a ballast resistor in the circuit,the discharge current is limited and the discharges remain in glow.The OH rotation temperature is obtained from fluorescence rotational branch fitting,and is about 350 K in pure water vapor.The effects of the discharge current and gas pressure on the production and quenching processes of OH radicals are investigated.The results show that in water vapor and He + H2O mixture gas the fluorescence intensity of OH stays nearly constant with increasing discharge current,and in N2 + H2O mixture gas the fluorescence intensity of OH increases with increasing discharge current.In water vapor and N2 + H2O mixture gas the fluorescence intensity of OH decreases with increasing gas pressure in the studied pressure range,and in He + H2O mixture gas the fluorescence intensity of OH shows a maximum value within the studied gas pressure range.The physicochemical reactions between electrons,radicals,ground and metastable molecules are discussed.The results in this work contribute to the optimization of plasma reactivity and the establishment of a molecule reaction dynamics model.     

In situ quantification of NO synthesis in a warm air glow discharge by WMS-based Mid-IR QCL absorption spectroscopy

Nitric oxide (NO) is one of the most crucial products in the plasma-based nitrogen fixation process. In this work, in situ measurements were performed for quantifying the NO synthesis spatially in a warm air glow discharge, through the method of Mid-infrared quantum cascade laser absorption spectroscopy (QCL-AS). Two ro-vibrational transitions at 1900.076 cm⁻¹ and 1900.517 cm⁻¹ of the ground-state NO(X) were probed sensitively by the help of the wavelength modulation spectroscopy (WMS) approach to increase the signal/noise (S/N) level. The results show a decline trend of NO synthesis rate along the discharge channel from the cathode to the anode. However, from the point of energy efficiency, the cathode region is of significantly low energy efficiency of NO production. Severe disproportionality was found for the high energy consumption but low NO production in the region of cathode area, compared to that in the positive column zone. Further analysis demonstrates the high energy cost of NO production in the cathode region, is ascribed to the extremely high reduced electric field $E/N$ therein not selectively preferable for the processes of vibrational excitation or dissociation of N₂ and O₂ molecules. This drags down the overall energy efficiency of NO synthesis by this typical warm air glow discharge, particularly for the ones with short electrode gaps. Limitations of further improving the energy cost of NO synthesis by variations of the discharge operation conditions, such as discharge current or airflow rate, imply other effective manners able to tune the energy delivery selectively to the NO formation process, are sorely needed.     

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.     

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.     

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.     

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.     

Spatio-temporal evolution characteristics and pattern formation of a gas–liquid interfacial AC current argon discharge plasma with a deionized water electrode

A discharge ignited by an AC power source in contact with deionized water as one of the electrodes is investigated. Immediately after initiation, the discharge exhibits a unique phenomenon: the gasphase discharge is extended into the liquid. Later, a cone-like structure is observed at the liquid surface. Synchronous monitoring of current–voltage characteristics and liquid properties versus time suggests that the discharge shapes are functions of the liquid properties. The spatio-temporal profiles indicate the potential effects of water, ambient air impurities, and metastable argon on the discharge chemistry. This becomes more obvious near the liquid surface due to increasing production of various transient reactive species such as ·OH and NO·. Moreover, it is revealed that thermalization of the rotational population distributions of the rotational states(N' ≤ 6,J'≤13/2) in the Q_1 branch of the OH(A~2∑~+,v'S=0→X~2∏_(3/2),v'=0 ) band ro-vibrational system is influenced by the humid environment near the liquid surface. In addition, the transient behaviors of instantaneous concentrations of long-lived reactive species(LRS) such as H_2O_2,NO_2~-, and-NO_3~- are observed with lengthening the discharge time. The production of multiple transient and LRS proposes AC excited gas–liquid argon discharge as a potential applicant in industrial wastewater cleaning, clinical medicine, and agriculture.     

Characteristic studies on positive and negative streamers of double-sided pulsed surface dielectric barrier discharge

The mechanisms of streamer generation and propagation in double-sided pulsed surface dielectric barrier discharge (SDBD) on both sides have been analyzed and investigated by experiment and numerical simulation. The fully exposed asymmetric SDBD has two discharge processes located on the high voltage electrode (HVE) side and the ground electrode (GE) side. Discharge images of the HVE side and GE side are taken by a digital camera under continuous pulse and ICCD (Intensified Charge Coupled Device) is utilized to diagnose the generation and propagation of streamers in single pulse discharge. In order to understand the physical mechanisms of streamer evolution more deeply, we establish a 2D simulation model and analyze it from the aspects of electron density, ion density, reduced electric field and electron impact ionization source term. The results show that the primary and secondary discharges on the HVE side and the GE side of the double-sided SDBD are composed of positive streamer and negative streamer, respectively. On the HVE side, the accumulation of positive charges on the dielectric surface causes the direction of the electric field to reverse, which is the principal factor for the polarity reversal of the streamer. On the GE side, both the negative charges accumulated on the dielectric surface and the falling voltage are the key factors for the streamer polarity switch.     

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.     

Three modes of a direct-current plasma jet operated underwater to degrade methylene blue

A direct-current air plasma jet operated underwater presents three stable modes including an intermittently-pulsed discharge, a periodically-pulsed discharge and a continuous discharge with increasing the power voltage. The three discharge modes have different appearances for the plasma plumes. Moreover, gap voltage-current characteristics indicate that the continuous discharge is in a normal glow regime. Spectral lines from reactive species(OH, N_2, N_2~+, H_α,and O) have been revealed in the emission spectrum of the plasma jet operated underwater.Spectral intensities emitted from OH radical and oxygen atom increase with increasing the power voltage or the gas flow rate, indicating that reactive species are abundant. These reactive species cause the degradation of the methylene blue dye in solution. Effects of the experimental parameters such as the power voltage, the gas flow rate and the treatment time are investigated on the degradation efficiency. Results indicate that the degradation efficiency increases with increasing the power voltage, the gas flow rate or the treatment time. Compared with degradation in the intermittently-pulsed mode or the periodically-pulsed one, it is more efficient in the continuous mode, reaching 98% after 21 min treatment.     

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.     

Removal of NO and SO2 in Corona Discharge Plasma Reactor with Water Film

In this paper, a novel type of a corona discharge plasma reactor was designed, which consists of needle-plate-combined electrodes, in which a series of needle electrodes are placed in a glass container filled with flue gas, and a plate electrode is immersed in the water. Based on this model, the removal of NO and SO2 was tested experimentally. In addition, the effect of streamer polarity on the reduction of SO2 and NO was investigated in detail. The experimental results show that the corona wind formed between the high-voltage needle electrode and the water by corona discharge enhances the cleaning efficiency of the flue gas because of the presence of water, and the cleaning efficiency will increase with the increase of applied dc voltage within a definite range. The removal efficiency of SO2 up to 98%, and about 85% of NO~ removal under suitable conditions is obtained in our experiments.     

Temporal Variation of the Current Sheet Inductance from PACO Plasma Focus Device

The temporal variation of the current sheet (CS) inductance in a plasma focus device can be calculated using the current derivative and the voltage signal acquired on the anode electrode, which are very common measurements in this type of device. The value of that inductance contains important information about the discharge performed including the CS lift-off from the insulator, voltage between the pinch extremes, maximum energy of the X-ray, energy delivered to the pinch and information about the actuating fusion mechanisms if the filling pressure is deuterium. This work discusses the values of the CS inductance extracted from several discharges of the Plasma Auto Confinado (PACO) plasma focus, installed in the National University of the Center of Buenos Aires—Argentina (2 kJ total energy, capacitor bank of 4 μF charged to 31 kV and a maximum current of 250 kA).