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.     

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.     

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.     

Novel Plasma Reactor with Rotary Helix Electrode Used in Coupling of CH4 at Atmospheric Pressure

At the ambient temperature and pressure a glow discharge plasma was used as a new approach for the coupling of methane with the newly-developed rotary multidentate helix electrode. In the presence of hydrogen, the effects of the input peak voltages and gas flow rates on methane conversion, C2 single pass yield and selectivity were investigated, and then the results were compared with those from the three-disc multidentate electrode. This demonstrated, on an experimental scale, that the rotary multidentate helix electrode was better than the multidentate three-disc electrode as there was little accumulation of coke, and the C2 yield per pass was 69.85% and C2 selectivity over 99.14% with 70.46% methane conversion at an input peak voltage of 2300 V and 60 ml/min gas flow rate.     

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.     

Electrical Characteristics of Pulsed Corona Discharge Plasmas in Chitosan Solution

Pulsed discharge plasma has exhibited active potential to prepare low molecular weight chitosan. In the present study, the viscosity of ehitosan solution was decreased noticeably after treated with pulsed corona discharge plasma. An experimental investigation on electrical characteristics of pulsed corona discharge plasma in chitosan solution was conducted with a view toward getting insight into discharge process. Factors affecting I-V curve, single pulse injec- tion energy and pulse width were studied. Experimental results showed positive effect of pulsed peak voltage on discharge plasma in chitosan solution. Pulse-forming capacitor greatly influenced the discharge form, and 4 nF was observed as a suitable value for efficiently generating stable discharge plasmas. As the electrode distance was larger than 10 ram, it had slight impact on dis- charge plasma due to the excellent conductive-property of chitosan solution. The injection energy significantly increased with air flow rate, while the pulse width hardly changed as the air flow rate increased from 0.5 m^3/h to 1.0 m^3/h. This study is expected to provide reference for promoting the application of pulsed corona discharge plasma to ehitosan solution treatment.     

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.     

Physicochemical properties of the AC-excited helium discharges using a water electrode

In this paper, the AC-excited helium discharges generated between the powered needle electrode enclosed in a conical quartz tube and the grounded de-ionized water electrode are investigated.The current and voltage waveforms exhibit a transition from the glow-like to streamer-like mode discharges, which forms a stable cone-shaped structure at the gas–liquid interface. In this region,the air and water vapor diffusion initiate various physical–chemical processes leading to substantial changes of the primary species emission intensities(e.g., OH, N_2, NO, and O) and the rotational temperatures. The experimentally measured rotational temperature at the gas–liquid interface is 870 K from the N_2(C–B) band with a power input of 26 W. With the prolongation of the discharge time, significant changes in the discharge voltage and current, discharge emission patterns, instantaneous concentrations of the secondary species(e.g., H_2O_2,NO_2~-, and NO_3~-) in the liquid phase, p H values and electrical conductivities of the liquids are observed experimentally. The present study is helpful for deepening the understandings to the basic physical–chemical processes in the discharges in contact with liquids, especially to those occurring in the vicinity of the gas–liquid interface, and also for promoting existing and potential applications of such type of discharges in the fields of environmental protection, biomedicine,agriculture, and so on.     

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.     

Degradation of antibiotic contaminants from water by gas–liquid underwater discharge plasma

Antibiotic contamination adversely affects human health and ecological balance.In this study,gasliquid underwater discharge plasma was employed to simultaneously degrade three antibiotics,sulfadiazine(SDZ),tetracycline(TC),and norfloxacin(NOR),to address the growing problem of antibiotic contaminants in water.The effects of various parameters on the antibiotic degradation efficiency were evaluated,including the discharge gas type and flow rate,the initial concentration and pH of the solution,and...     

Degradation of tiamulin by a packed bed dielectric barrier plasma combined with TiO2 catalyst

Recently, a plasma catalyst was employed to efficiently degrade antibiotic residues in the environment. In this study, the plasma generated in a packed bed dielectric barrier reactor combined with TiO2 catalyst is used to degrade the antibiotic tiamulin (TIA) loaded on the surface of simulated soil particles. The effects of applied voltage, composition of the working gas, gas flow rate and presence or absence of catalyst on the degradation effect were studied. It was found that plasma and catalyst can produce a synergistic effect under optimal conditions (applied voltage 25 kV, oxygen ratio 1%, gas flow rate 0.6 l min−1, treatment time 5 min). The degradation efficiency of the plasma combined with catalyst can reach 78.6%, which is 18.4% higher than that of plasma without catalyst. When the applied voltage is 30 kV, the gas flow rate is 1 l min−1, the oxygen ratio is 1% and the plasma combined with TiO2 catalyst treats the sample for 5 min the degradation efficiency of TIA reached 97%. It can be concluded that a higher applied voltage and longer processing times not only lead to more degradation but also result in a lower energy efficiency. Decreasing the oxygen ratio and gas flow rate could improve the degradation efficiency. The relative distribution and identity of the major TIA degradation product generated was determined by high-performance liquid chromatography–mass spectrometry analysis. The mechanism of TIA removal by plasma and TiO2 catalyst was analyzed, and the possible degradation path is discussed.     

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.     

Experimental study on plasma actuation characteristics of nanosecond pulsed dielectric barrier discharge

Combining high-speed schlieren technology and infrared imaging technology, related research has been carried out on the influence of parameters such as actuation voltage, repetition frequency, and electrode size of an actuator on the discharge characteristics, induced flow field characteristics, and thermal characteristics of nanosecond pulsed dielectric barrier discharge. The results show that increasing the value of the actuation voltage can significantly increase the actuation intensity, and the plasma discharge area is significantly extended. Increasing the repetition frequency can increase the number of discharges per unit time. Both will cause more energy input and induce more changes in the flow field. The effect of temperature rise is more significant. The width of the covered electrode will affect the potential distribution during the discharge process, which in turn will affect the extension process of the plasma discharge filament. Under the same actuation intensity, the wider the covered electrode, the larger range the induced flow field and temperature rise is. Preliminary experimental analyses of high-frequency actuation characteristics, temperature field characteristics, flow field characteristics and actuation parameter settings provide support for the parameter selection and partial mechanism analysis of plasma anti-icing.     

Spatiotemporal control of femtosecond laser filament-triggered discharge and its application in diagnosing gas flow fields

Precise control of the discharge in space and time is of great significance for better applications of discharge plasma. Here, we used a femtosecond laser filament to trigger and guide a high-voltage DC pulse discharge to achieve spatiotemporal control of the discharge plasma. In space, the discharge plasma is distributed strictly along the channel generated by the femtosecond laser filament. The breakdown voltage threshold is reduced, and the discharge length is extended. In time, the electrical parameters such as the electrode voltage and the electrode gap affect discharge delay time and jitter. By optimizing the parameters, we can achieve sub-nanosecond jitter of the discharge. Based on the spatiotemporal control of the discharge, we applied filament-triggered discharge for one-dimensional composition measurements of the gas flow field. Besides, the technique shows great potential in studying the spatiotemporal evolution of discharge plasma.     

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 Effect of Gas Flow Rate on Radio-Frequency Hollow Cathode Discharge Characteristics

It is known that gas flow rate is a key factor in controlling industrial plasma processing. In this paper, a 2D PIC/MCC model is developed for an rf hollow cathode discharge with an axial nitrogen gas flow. The effects of the gas flow rate on the plasma parameters are calculated and the results show that： with an increasing flow rate, the total ion（N＋2, N＋） density decreases, the mean sheath thickness becomes wider, the radial electric field in the sheath and the axial electric field show an increase, and the energies of both kinds of nitrogen ions increase;and, as the axial ion current density that is moving toward the ground electrode increases, the ion current density near the ground electrode increases. The simulation results will provide a useful reference for plasma jet technology involving rf hollow cathode discharges in N2.     

Temperature dependence of pattern transitions on water surface in contact with DC microplasmas

The DC-driven atmospheric-pressure microplasma is generated in a helium gas flowing through the metal tube cathode and is brought into contact with the surface of the water with the immersed Pt anode. By adjusting the gas flow, discharge current and gap distance, self-organized patterns are observed and varied sequentially from the homogeneous spot to the ring-like shape,distinct spot shape and the gearwheel shape on the water surface. The electrode temperature is measured and the gas temperature of the plasma discharge is calculated through the numericalfitting of the second positive system of the spectrum of N2 molecules. It is shown that the pattern transition is related to the electrode and gas temperatures of the plasma. Moreover, specific discretization features of the patterns are shown to appear at certain gas temperatures.     

Dynamics of plasma bullets by nanosecond pulsed micro-hollow cathode discharge within air

In this paper, the air plasma jet produced by micro-hollow cathode discharge(MHCD) is investigated. The discharge is powered by a positive nanosecond pulse high voltage supply. The waveforms of the discharge, the images of the jet, the evolution of the plasma bullet and the reactive species are obtained to analyze the characteristics of the MHCD plasma jet. It is found that the length of the plasma jet is almost proportional to the air flow rate of 2–6 slm. Two plasma bullets appear one after another during a single period of the voltage waveform, and both of the two plasma bullets are formed during the positive pulse voltage off. The propagation velocity of the two plasma bullets is on the order of several hundred m/s, which is approximate to that of the air flow. These results indicate that the gas flow has an important influence on the formation of this MHCD plasma jet.     

The influence of grounded electrode positions on the evolution and characteristics of an atmospheric pressure argon plasma jet

An atmospheric pressure plasma jet (APPJ) in Ar with various grounded electrode arrangements is employed to investigate the effects of electrode arrangement on the characteristics of the APPJ.Electrical and optical methods are used to characterize the plasma properties.The discharge modes of the APPJ with respect to applied voltage are studied for grounded electrodepositions of 10 mm,40 mm and 80 mm,respectively,and the main discharge and plasma parameters are investigated.It is shown that an increase in the distance between the grounded electrode and high-voltage electrode results in a change in the discharge modes and discharge parameters.The discharges transit from having two discharge modes,dielectric barrier discharge (DBD) and jet,to having three,corona,DBD and jet,with increase in the distance from the grounded to the high-voltage electrodes.The maximum length of the APPJ reaches 3.8 cm at an applied voltage of 8 kV.The discharge power and transferred charges and spectral line intensities for species in the APPJ are influenced by the positions of the grounded electrode,while there is no obvious difference in the values of the electron excited temperature (EET) for the three grounded electrode positions.     

Synthesis of Cu-Doped Mixed-Phase TiO2 with the Assistance of Ionic Liquid by Atmospheric-Pressure Cold Plasma

An atmospheric-pressure dielectric barrier discharge(DBD) gas-liquid cold plasma was employed to synthesize Cu-doped TiO_2 nanoparticles in an aqueous solution with the assistance of[C_2MIM]BF_4 ionic liquid(IL) and using air as the working gas.The influences of the discharge voltage,IL and the amount of copper nitrite were investigated.X-ray diffraction,N_2adsorption-desorption measurements and UV-Vis spectroscopy were adopted to characterize the samples.The results showed that the specific surface area of TiO_2 was promoted with Cu-doping(from 57.6 m~2·g~(-1) to 106.2 m~2·g~(-1) with 3%Cu-doping),and the content of anatase was increased.Besides,the band gap energy of TiO_2 with Cu-doping decreased according to the UV-Vis spectroscopy test.The 3%Cu-IL-TiO_2 samples showed the highest efficiency in degrading methylene blue(MB) dye solutions under simulated sunlight with an apparent rate constant of 0.0223 min~(-1),which was 1.2 times higher than that of non-doped samples.According to the characterization results,the reasons for the high photocatalytic activity were discussed.