Regulation characteristics of oxide generation and formaldehyde removal by using volume DBD reactor

Discharge plasmas in air can be accompanied by ultraviolet(UV) radiation and electron impact,which can produce large numbers of reactive species such as hydroxyl radical(OH·),oxygen radical(O·),ozone(O3),and nitrogen oxides(NOx),etc.The composition and dosage of reactive species usually play an important role in the case of volatile organic compounds(VOCs) treatment with the discharge plasmas.In this paper,we propose a volume discharge setup used to purify formaldehyde in air,which is configured by a plate-to-plate dielectric barrier discharge(DBD) channel and excited by an AC high voltage source.The results show that the relative spectral-intensity from DBD cell without formaldehyde is stronger than the case with formaldehyde.The energy efficiency ratios(EERs) of both oxides yield and formaldehyde removal can be regulated by the gas flow velocity in DBD channel,and the most desirable processing effect is the gas flow velocity within the range from2.50 to 3.33 m s-1.Moreover,the EERs of both the generated dosages of oxides(O3 and NO2) and the amount of removed formaldehyde can also be regulated by both of the applied voltage and power density loaded on the DBD cell.Additionally,the EERs of both oxides generation and formaldehyde removal present as a function of normal distribution with increasing the applied power density,and the peak of the function is appeared in the range from 273.5 to 400.0 W l-1.This work clearly demonstrates the regulation characteristic of both the formaldehyde removal and oxides yield by using volume DBD,and it is helpful in the applications of VOCs removal by using discharge plasma.     

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.     

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.     

Characteristics of Single Cathode Cascaded Bias Voltage Arc Plasma

A single cathode with a cascaded bias voltage arc plasma source has been developed with a new quartz cathode chamber,instead of the previous copper chambers,to provide better diagnostic observation and access to the plasma optical emission.The cathode chamber cooling scheme is also modified to be naturally cooled only by light emission without cooling water to improve the optical thin performance in the optical path.A single-parameter physical model has been developed to describe the power dissipated in the cascaded bias voltage arc discharge argon plasmas,which have been investigated by utilizing optical emission spectroscopy(OES) and Langmuir probe.In the experiments,discharge currents from 50 A to 100 A,argon flow rates from 800 sccm to 2000 sccm and magnetic fields of 0.1 T and 0.2 T were chosen.The results show:(a) the relationship between the averaged resistivity and the averaged current density exhibits an empirical scaling law as η∝ j~(-0.63369) and the power dissipated in the arc has a strong relation with the filling factor;(b) through the quartz,the argon ions optical emission lines have been easily observed and are dominating with wavelengths between 340 nm and 520 nm,which are the emissions of Ar~+-434.81 nm and Ar~+-442.60 nm line,and theintensities are increasing with the arc current and decreasing with the inlet argon flow rate;and(c) the electron density and temperature can reach 2.0 × 10~(19) m~(-3) and 0.48 eV,respectively,under the conditions of an arc current of 90 A and a magnetic field of 0.2 T.The half-width of the n_e radial profile is approximatively equal to a few Larmor radii of electrons and can be regarded as the diameter of the plasma jet in the experiments.     

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.     

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.     

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.     

Numerical Modelling and Simulation of Chemical Reactions in a Nano-Pulse Discharged Bubble for Water Treatment

A zero-dimensional model to simulate a nano-pulse-discharged bubble in water was developed.The model consists of gas and liquid phases corresponding to the inside and outside of the bubble,respectively.The diffusions of chemical species from the gas to the liquid phase through the bubble interface was also investigated.The initial gas is Ar,but includes a little H_2O and O2 in the bubble.The time evolution of the OH concentration in the liquid phase was mainly investigated as an important species for water treatment.It was shown that OH was generated in the bubble and then diffused into the liquid.With the application of a continuous nano-pulse discharge,more OH radicals were generated as the frequency increased at a low voltage for a given power consumption.     

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.     

Study of Non-Thermal DC Arc Plasma of CH_4/Ar at Atmospheric Pressure Using Optical Emission Spectroscopy and Mass Spectrometry

Non-thermal C/H/Ar plasmas are widely applied to carbonaceous material production and processing.In this work,plasma parameters and gaseous species of the atmospheric non-thermal C/H/Ar plasmas produced by an atmospheric-pressure DC arc discharge generator in CH_4/Ar were investigated.The voltage-current characteristics were measured for different CH_4/Ar ratios.Optical emission spectroscopy was employed to analyze the electron excitation temperature,gas temperature and electron density under various discharge conditions.The hydrocarbon molecules produced in the CH_4/Ar plasmas were detected with photoionization mass spectrometry.The optical spectral results demonstrated that the electron excitation temperature was 0.4-1 eV,the gas temperature was 2800-4200 K and the electron density was in the range of(5-20)×10~(15) cm~(-3).The mass spectrum indicated that a variety of unsaturated hydrocarbons(C_2H_4,C_3H_6,C_6H_6,etc.) and several highly unsaturated hydrocarbons(C_4H_2,C_5H_6,etc.) were produced in the non-thermal arc plasmas.     

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.     

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.     

Experimental study on toluene removal by a two-stage plasma-biofilter system

Volatile organic compounds (VOCs) are typical pollutants that affect air quality. Discharge plasma is thought to be a potential method that can remove VOCs from flue gas. In this experiment, pulsed corona discharge plasma combined with a biological tower was carried out to remove the benzene series, and toluene was selected as the typical VOC. The results indicated that the removal efficiency of toluene by pulsed corona plasma was slightly higher than that of direct current (DC) corona plasma, while its energy efficiency was much higher than DC corona plasma. Under the optimal experimental conditions of pulse voltage 8.5 kV, initial toluene concentration 1400 mg m−3, and toluene flow rate of 12 l h−1, the toluene removal efficiency reached 77.11% by the single method of pulsed corona discharge plasma, and the energy efficiency was up to 1.515 g/(kW·h) under the pulse voltage of 4.0 kV. The trickling biofilter was constructed by using the screened and domesticated Acinetobacter baumannii, and the highest toluene removal efficiency by the pulsed corona discharge plasma combined with the trickling biofilter rose up to 97.84%. Part of the toluene was degraded into CO2, H2O, and some intermediate products such as o-diphenol under the influence of Acinetobacter baumannii. When the remaining waste gas passed through the discharge plasma reactor, the benzene ring structure could be directly destroyed by the collision between toluene and plasma. Meanwhile, O·, OH·, and some other oxidizing radicals generated by the discharge also join into the oxidative decomposition of toluene and its intermediate products, thereby further improving the removal efficiency of toluene. Therefore, the two-stage plasma-biofilter system not only showed a high toluene removal efficiency, but also had a good energy efficiency. The results of this study will provide theoretical support and technical reference for industrial VOC treatment.     

Optical Spectroscopic Investigation of Ar/CH_3OH and Ar/N_2/CH_3OH Atmospheric Pressure Plasma Jets

Ar/CH3OH and Ar/N2/CH3OH plasma jets were generated at atmospheric pressure by dual-frequency excitations. Two different cases were studied with focus laid on the generation of CN radicals. In one case Ar gas passed through a bubbler with saturated methanol steam but without addition of N2 （Ar/CH3OH plasma）. In the other case N2 passed through the bubbler with saturated methanol steam （Ar/N2/CH3OH plasma）. The optical emission lines of CN radicals have been observed in these two cases of plasma discharges. The addition of N2 can significantly increase the optical emission intensity of CN bands.     

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.     

Conversion of coalbed methane surrogate into hydrogen and graphene sheets using rotating gliding arc plasma

The use of atmospheric rotating gliding arc(RGA) plasma is proposed as a facile, scalable and catalyst-free approach to synthesizing hydrogen(H_2) and graphene sheets from coalbed methane(CBM). CH_4 is used as a CBM surrogate. Based on a previous investigation of discharge properties, product distribution and energy efficiency, the operating parameters such as CH_4 concentration, applied voltage and gas flow rate can effectively affect the CH_4 conversion rate,the selectivity of H_2 and the properties of solid generated carbon. Nevertheless, the basic properties of RGA plasma and its role in CH_4 conversion are scarcely mentioned. In the present work, a 3D RGA model, with a detailed nonequilibrium CH_4/Ar plasma chemistry, is developed to validate the previous experiments on CBM conversion, aiming in particular at the distribution of H_2 and other gas products. Our results demonstrate that the dynamics of RGA is derived from the joint effects of electron convection, electron migration and electron diffusion, and is prominently determined by the variation of the gas flow rate and applied voltage. Subsequently,a combined experimental and chemical kinetical simulation is performed to analyze the selectivity of gas products in an RGA reaction, taking into consideration the formation and loss pathways of crucial targeted substances(such as CH_4, C_2H_2, H_2 and H radicals) and corresponding contribution rates. Additionally, the effects of operating conditions on the properties of solid products are investigated by scanning electron microscopy(SEM) and Raman spectroscopy. The results show that increasing the applied voltage and decreasing CH_4 concentration will change the solid carbon from its initial spherical structure into folded multilayer graphene sheets, while the size of the graphene sheets is slightly affected by the change in gas flow rate.     

Asphaltene Erosion Process in Air Plasma: Emission Spectroscopy and Surface Analysis for Air-Plasma Reactions

Optical emission spectroscopy (OES) was applied for plasma characterization during the erosion of asphaltene substrates. An amount of 100 mg of asphaltene was carefully applied to an electrode and exposed to air-plasma glow discharge at a pressure of 1.0 Torr. The plasma was generated in a stainless steel discharge chamber by an ac generator at a frequency of 60 Hz, output power of 50 W and a gas flow rate of 1.8 L/min. The electron temperature and ion density were estimated to be 2.15±0.11 eV and (1.24±0.05)×1016 m-3 , respectively, using a double Langmuir probe. OES was employed to observe the emission from the asphaltene exposed to air plasma. Both molecular band emission from N2 , N+2 , OH, CH, NH, O2 as well as CN, and atomic light emission from V and Hγ were observed and used to monitor the evolution of asphaltene erosion. The asphaltene erosion was analyzed with the aid of a scanning electron microscope (SEM) equipped with an energy dispersive X-ray (EDX) detector. The EDX analysis showed that the time evolution of elements C, O, S and V were similar; and the chemical composition of the exposed asphaltenes remained constant. Particle size evolution was measured, showing a maximum size of 2307 μm after 60 min. This behavior is most likely related to particle agglomeration as a function of time.     

Nonequilibrium Atmospheric Pressure Ar/O2 Plasma Jet: Properties and Application to Surface Cleaning

In this study an atmospheric pressure Ar/O_2 plasma jet is generated to study the effects of applied voltage and gas flux rate to the behavior of discharge and the metal surface cleaning.The increase in applied voltage leads to increases of the root mean square(rms) current,the input power and the gas temperature.Furthermore,the optical emission spectra show that the emission intensities of metastable argon and atomic oxygen increase with increasing applied voltage.However,the increase in gas flux rate leads to a reduction of the rms current,the input power and the gas temperature.Furthermore,the emission intensities of metastable argon and atomic oxygen decrease when gas flux rate increases.Contact angles are measured to estimate the cleaning performance,and the results show that the increase of applied voltage can improve the cleaning performance.Nevertheless,the increase of gas flux rate cannot improve the cleaning performance.Contact angles are compared for different input powers and gas flux rates to search for a better understanding of the major mechanism for surface cleaning by plasma jets.     

Influence of water vapor concentration on discharge dynamics and reaction products of underwater discharge within a He/H_2O-filled bubble at atmospheric pressure

In this study, a two-dimensional fluid model is proposed to simulate the underwater discharge in a He/H_2O-filled bubble at atmospheric pressure. The molar fraction of water vapor is varied in the range of 0.01%–1% to investigate the dependence of discharge dynamics and reaction products on water vapor concentration(WVC). The numerical results show that most properties of the discharge sensitively depend on the WVC. The increase of WVC leads to an increase in the electron density and discharge propagation velocity, which is attributed to Penning ionization between He*and H_2O. The main positive ion switches from He+to H_2O~+, while the WVC increases from 0.01% to 1%. The dominant reactive oxygen species is OH, whose peak density is about two orders of magnitude higher than that of O. Besides, the densities of OH and O radicals increase with the increasing WVC. It is shown that the formation mechanism of O radicals is significantly affected by the WVC. The dominant reaction creating O radicals changes from the charge exchange between He+2 and H_2O to the electron impact dissociation of H_2O as the WVC increases from 0.01% to 1%. This study is helpful for better understanding the application of non-thermal plasmas discharges in water, such as biomedical, environmental engineering.     

Dynamic behavior of a rotating gliding arc plasma in nitrogen: effects of gas flow rate and operating current

The effects of feed gas flow rate and operating current on the electrical characteristics and dynamic behavior of a rotating gliding arc (RGA) plasma codriven by a magnetic field and tangential flow were investigated.The operating current has been shown to significantly affect the time-resolved voltage waveforms of the discharge,particularly at flow rate =21 min-1.When the current was lower than 140 mA,sinusoidal waveforms with regular variation periods of 13.5-17.0 ms can be observed (flow rate =21 min-1).The restrike mode characterized by serial sudden drops of voltage appeared under all studied conditions.Increasing the flow rate from 8 to 121 min-1 (at the same current) led to a shift of arc rotation mode which would then result in a significant drop of discharge voltage (around 120-200 V).For a given flow rate,the reduction of current resulted in a nearly linear increase of voltage.