Development of low power non-thermal plasma jet and optimization of operational parameters for treating dyes and emerging contaminants

Non-thermal plasma has emerged as an effective treatment system against the latest class of highly recalcitrant and toxic environmental pollutants termed emerging contaminants (ECs). In the present work, a detailed experimental study is carried out to evaluate the efficacy of a non-thermal plasma jet with two dyes, Rd. B and Met. Blue, as model contaminants. The plasma jet provided a complete dye decoloration in 30 min with an applied voltage of 6.5 kV_p−p. ·OH, having the highest oxidation potential, acts as the main reactive species, which with direct action on contaminants also acts indirectly by getting converted into H2O2 and O3. Further, the effect of critical operational parameters viz, sample pH, applied voltage (4.5‒6.5 kV_p−p), conductivity (5‒20 mS cm⁻¹), and sample distance on plasma treatment efficacy was also examined. Out of all the assessed parameters, the applied voltage and sample conductivity was found to be the most significant operating parameters. A high voltage and low conductivity favored the dye decoloration, while the pH effect was not that significant. To understand the influence of plasma discharge gas on treatment efficacy, all the experiments are conducted with argon and helium gases under the fixed geometrical configuration. Both the gases provided a similar dye decoloration efficiency. The DBD plasma system with complete dye removal also rendered maximum mineralization of 73% for Rd. B, and 60% for Met. Blue. Finally, the system's efficiency against the actual ECs (four pharmaceutical compounds, viz, metformin, atenolol, acetaminophen, and ranitidine) and microbial contaminant (E. coli) was also tested. The system showed effectivity in the complete removal of targeted pharmaceuticals and a log2.5 E. coli reduction. The present systematic characterization of dye degradation could be of interest to large communities working towards commercializing plasma treatment systems.     

Degradation of Aniline Wastewater Using Dielectric Barrier Discharges at Atmospheric Pressure

Aniline is a toxic water pollutant detected in drinking water and surface water,and this chemical is harmful to both human and aquatic life.A dielectric barrier discharge(DBD)reactor was designed in this study to investigate the treatment of aniline in aqueous solution.Discharge characteristics were assessed by measuring voltage and current waveforms,capturing light emission images,and obtaining optical emission spectra.The effects of several parameters were analyzed,including treatment distance,discharge power,DBD treatment time,initial pH of aniline solutions,and addition of sodium carbonate and hydrogen peroxide to the treatment.Aniline degradation increased with increasing discharge power.Under the same conditions,higher degradation was obtained at a treatment distance of 0 mm than at other treatment distances.At a discharge power of 21.5 W,84.32%of aniline was removed after 10 min of DBD treatment.Initial pH significantly influenced aniline degradation.Adding a certain dosage of sodium carbonate and hydrogen peroxide to the wastewater can accelerate the degradation rate of aniline.Possible degradation pathways of aniline by DBD plasmas were proposed based on the analytical data of GC/MS and TOC.     

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.     

Activated persulfate by DBD plasma and activated carbon for the degradation of acid orange Ⅱ

In this study, the effect of activated peroxydisulfate(PDS) by dielectric barrier discharge(DBD) plasma and activated carbon(HGAC) on the removal of acid orange Ⅱ(AOⅡ) was investigated. The effects of applied voltage, PDS dosage, HGAC dosage, initial pH value, and inorganic anions on the removal rate of AOⅡ were discussed. The main free radicals degrading azo dyes during the experiment were also studied. Experimental results show that the removal rate of AOⅡ in DBD/HGAC/PDS synergistic system is much higher than that in the single system. With the applied voltage of 16 kV, HGAC dosage of 1 g l-1, PDS and AOⅡ molar ratio of 200:1, initial pH value of 5.4 and concentration of AOⅡ solution of 20 mg l-1, the removal rate of AOⅡ reached 97.6% in DBD/HGAC/PDS process after 28 min of reaction.Acidic and neutral conditions are beneficial for AOⅡ removal. Sulfate and hydroxyl radicals play an important role in the removal of AOⅡ. Inorganic anions are not conducive to the removal of AOⅡ.     

Treatment of Wastewater with High Conductivity by Pulsed Discharge Plasma

A wastewater treatment system was established by means of pulsed dielectric barrier discharge（DBD）. The main advantage of this system is that the wastewater is employed as one of the electrodes for the degradation of rhodamine B, which makes use of the high conductivity and lessenes its negative influence on the discharge process. At the same time, the reactive species like ozone and ultraviolet（UV） light generated by the DBD can be utilized for the treatment of wastewater. The effects of some factors like conductivity, peak pulse voltage, discharge frequency and pH values were investigated. The results show that the combination of these reactive species could enhance the degradation of the dye while the ozone played the most important role in the process. The degradation efficiency was enhanced with the increase of energy supplied. The reduction in the concentration of rhodamine B was much more effective with high solution conductivity;under the highest conductivity condition, the degradation rate could rise to 99%.     

Experimental Research on the Sterilization of Escherichia Coli and Bacillus Subtilis in Drinking Water by Dielectric Barrier Discharge

The bactericidal effect on the representative type of Gram-negative Escherichia coli(E.coli) and Gram-positive Bacillus subtilis in drinking water was investigated in this paper by using dielectric barrier discharge(DBD) advanced oxidation technology.The sterilizing rates under different conditions of reaction time t,input voltage V,p H value,and initial concentration of bacteria C_0 were investigated to figure out the optimum sterilization conditions.Our observations and comparisons of cell morphology alteration by scanning electron microscopy and transmission electron microscopy revealed the sterilization mechanisms.The results showed that the sterilizing rate increased obviously with the extension of reaction time t and the rise of input voltage V.The optimal sterilization effect was achieved when the p H value was 7.1.As the initial concentration of bacteria rose,the sterilizing rate decreased.When the input voltage was 2.2 k V and the initial concentration of bacteria was relatively low,the sterilizing rate almost reached 100% after a certain treatment time in neutral aqueous solution.The reasons for the great damage of cell structure and the killing of bacteria are the oxidation of O_3,OH and the accumulation of active species produced by DBD.The article provides a certain theoretical and experimental basis for DBD application in water pollution treatment.     

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.     

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.     

High concentration xylene decomposition and diagnostic analysis by non-thermal plasma in a DBD reactor

Dielectric barrier discharge (DBD) is utilized to decompose xylene vapor in mobile gas under normal atmospheric pressure.The plasma is generated by an AC power source with a frequency of 6 kHz.In the experiment,the discharge power on the DBD reactor was calculated by a Lissajous figure,and the specific input energy (SIE) of different discharge voltage or residence time was obtained.The concentrations of xylene,carbon monoxide and carbon dioxide in the gas were analyzed by gas chromatography.The spectra of DBD were diagnosed using a spectrometer.We calculated the conversion rate (CR),mineralization rate (MR) and carbon dioxide selectivity.The relationship between these quantities and the SIE was analyzed.The experimental results show that high concentration xylene can be decomposed mostly by DBD plasma.The CR can reach as high as 90％ with the main product of carbon dioxide.     

Parameter Optimization for Enhancement of Ethanol Yield by Atmospheric Pressure DBD-TreatedSaccharomyces cerevisiae简

In this study, Saccharomyces cerevisiae （S. cerevisiae） was exposed to dielectric barrier discharge plasma （DBD） to improve its ethanol production capacity during fermenta- tion. Response surface methodology （RSM） was used to optimize the discharge-associated pa- rameters of DBD for the purpose of maximizing the ethanol yield achieved by DBD-treated S. cerevisiae. According to single factor experiments, a mathematical model was established using Box-Behnken central composite experiment design, with plasma exposure time, power supply volt- age, and exposed-sample volume as impact factors and ethanol yield as the response. This was followed by response surface analysis. Optimal experimental parameters for plasma discharge- induced enhancement in ethanol yield were plasma exposure time of 1 rain, power voltage of 26 V, and an exposed sample volume of 9 mL. Under these conditions, the resulting yield of ethanol was 0.48 g/g, representing an increase of 33% over control.     

Effect of Atmospheric Pressure Plasma Treatment/Followed by Chitosan Grafting on Antifelting and Dyeability of Wool Fabric

Effect of chitosan on antifelting and dyability of dielectric barrier discharge (DBD) pretreated wool fabric were evaluated. We have used a DBD, working in an atmospheric pressure air for pretreatment of wool fabric. The chitosan was applied to pretreated wool fabrics by using pad-dry cure technique. The anti-felting properties of the wool samples were studied and it was shown that the shrink resistance and anti-felting behavior of the wool had been significantly improved by the DBD pretreatment followed by chitosan grafting. In addition, dye ability of wool fabrics after plasma/chitosan treatment is improved. Some analytical skills such as Fourier transform infrared spectroscopy and scanning electron microscope were used to characterize the different aspects of the treated fabric.     

Simulated and experimental studies on the array dielectric barrier discharge of water electrodes

A kind of dielectric barrier discharge(DBD) device composed of water electrodes with 3×3forms can produce large-area low-temperature plasmas at atmospheric pressure.To reflect the discharge characteristics of DBD better,a dynamic simulation model,which is based on the voltage controlled current source(CCS),is established,then the established model in Matlab/Simulink is used to simulate the DBD in air.The voltage-current waves and Lissajous at a voltage of 10 kV,11 kV and 12 kV peak value with a frequency of 15 kHz are studied.The change of the discharge power of DBD with a different amplitude and frequency of applied voltage is also analyzed.The result shows the voltage-current waves,Lissajous and discharge power of DBD under different conditions from the simulation agree well with those of the experiment.In addition,we propose a method to calculate the dielectric barrier capacitance C_d and the gap capacitance C_g,which is valid through analyzing the variation of capacitance at different voltage amplitudes.     

Investigation of operating parameters on CO2 splitting by dielectric barrier discharge plasma

Experiments of CO2 splitting by dielectric barrier discharge (DBD) plasma were carried out,and the influence of CO2 flow rate,plasma power,discharge voltage,discharge frequency on CO2 conversion and process energy efficiency were investigated.It was shown that the absolute quantity of CO2 decomposed was only proportional to the amount of conductive electrons across the discharge gap,and the electron amount was proportional to the discharge power;the energy efficiency of CO2 conversion was almost a constant at a lower level,which was limited by CO2 inherent discharge character that determined a constant gap electric field strength.This was the main reason why CO2 conversion rate decreased as the CO2 flow rate increase and process energy efficiency was decreased a little as applied frequency increased.Therefore,one can improve the CO2 conversion by less feed flow rate or larger discharge power in DBD plasma,but the energy efficiency is difficult to improve.     

The Degradation of Organic Pollutants by Bubble Discharge in Water

Organic pollutants could be degraded by using bubble discharge in water with gas aeration in the discharge reactor and more plasma can be generated in the discharge process.When pulsed high voltage was applied between electrodes with gas aerated into the reactor,it showed that bubbles were broken,which meant that breakdown took place.It could also be observed that the removal rate of phenol increased with increasing discharge voltage or pulse frequency,and with reducing initial phenol concentration or solution electric conductivity.It could remove more amount of phenol by oxygen aeration.With increasing oxygen flow rate,the removal rate increased.There was little difference with air or nitrogen aeration for phenol removal.The solution temperature after discharge increased to a great extent.However,this part of energy consumption did not contribute to the reaction,which led to a reduction in the energy utilization efficiency.     

An Experimental Study on Atmospheric Pressure Glow Discharge in Different Gases

Usually,the electrical breakdown of dielectric barrier discharge(DBD) at atmospheric pressure leads to a filamentary non-homogeneous discharge,However,it is also possible to obtain a diffuse DBD in homogeneous form,called atmospheric pressure glow discharge(APGD).We obtained a uniform APGD in helium and in the mixture of argon with alcohol,and studied the electrical characteristics of helium APGD.It if found that the relationship between discharge current and source frequency is different depending on the difference in gas gap when the applied voltage is kept constant.The discharge current shows an increasing trend with the increased frequency when gas gap is 0.8cm ,but the discharge current tends to decrease with the increased frequency when the gas gap increases.The discharge current always increases with the increased applied voltage when the source frequency is kept constant.We also observed a glow-like discharge in nitrogen at atmospheric pressure.     

Application of DBD and DBCD in SO2 Removal

The dielectric barrier corona discharge(DBCD) in a wire-cylinder configuration and the dielectric barrier discharge(DBD) in a coaxial cylinder configuration are studied. The discharge current in DBD has a higher pulse amplitude than in DBCD. The dissipated power and the gas-gap voltage are calculated by analyzing the measured Lissajous figure. With the increasing applied voltage, the energy utilization factor for SO2 removal increases in DBCD but decreases in DBD because of the difference in their electric field distribution. Experiments of SO2 removal show that in the absence of NH3 the energy utilization factor can reach 31 g/kWh in DBCD and 39 g/kWh in DBD.     

On surface elementary processes and polymer surface modifications induced by double pulsed dielectric barrier discharge

In this paper, polyethylene terephthalate and polyethylene films were plasma treated using a dielectric barrier discharge (DBD), which presents a second current pulse with inverse polarity induced at the decreasing applied voltage flank in addition to the main current pulse. The surface modifications of polymer samples were pointed out by two complementary methods: the contact angle method and atomic force microscopy (AFM) technique. The influence of the voltage pulse parameters as width, falling rate and frequency on the secondary discharge formation was studied and correlated with polymer surface modifications. The plasma treatment is improved when the discharge is driven by a voltage pulses with very fast falling flank. After plasma treatment, roughness of the PE films is not considerably changed; only topographical modifications of PE treated samples being observed, while treated PET surfaces present an increased roughness and a new granular structure, with much smaller features compared to the pristine ones.     

Improving the surface insulation of epoxy resin by plasma etching

Epoxy resin (EP) tends to accumulate a large amount of charge on its surface when exposed to a high-voltage DC electric field,which leads to a reduction in its insulative performance and an increase in potential safety risks in power systems.To suppress charge accumulation,improve the flashover voltage of the EP,and reduce the risk of gas insulated switchgear (GIS)/gas insulated transmission line (GIL) failure,we used two plasma-etching methods,i.e.,atmospheric-pressure dielectric barrier discharge (DBD) and the atmospheric-pressure plasma jet(APPJ),to modify the surface of the EP.The surface morphology and electrical properties of the modified materials were explored as a function of time.The results show that after DBD treatment,the roughness of the sample increases by 103.9 nm,the conductivity increases by3.9?×?10~(–18)S,and the flashover voltage increases by 14.4%;after APPJ treatment,the roughness of the sample increases by 223.5 nm,the conductivity increases by 3.4?×?10~(–17)S,and the flashover voltage increases by 18%.This shows that both plasma-etching methods can improve the insulation properties of materials by improving the surface-charge characteristics.The two methods are compared with each other:the APPJ treatment method is better at improving the surface roughness and electrical properties of materials,and this flexible treatment method has greater potential in industrial applications.     

Study on the properties of a ε-Fe3N-based magnetic lubricant prepared by DBD plasma

The ε-Fe₃N-based magnetic lubricant which is stable and high saturation magnetization has been prepared by a homemade DBD device under the atmospheric pressure. The results show that the NH3 flow rate, the applied peak-to-peak voltage and the mass ratio of surfactant and carrier lubricant have important effects on the phase structure, the magnetic properties, the size of ferroparticles and the stability of the ε-Fe3N-based magnetic lubricant. TEM images show the ε-Fe₃N ferroparticles are dispersed in the carrier lubricant homogeneously, and the cluster phenomenon is not observed. The stable ε-Fe3N-based magnetic lubricant with the saturation magnetization of 50.11 mT and the mean ferroparticle size of 11 nm is prepared successfully. The main particles of the atmospheric-pressure Ar/NH3/Fe(CO)5 DBD plasma are NH, N, N⁺, Fe, N₂, Ar, H_α, and CO; NH is a decomposition product of NH₃. Fe and N active radicals are two elementary species in the preparation of the ε-Fe3N-based magnetic lubricant in the atmospheric-pressure DBD plasma. There are two discharge modes for DBD plasma, namely, multi-pulse APGD and filamentary discharge. By increasing the applied peak-to-peak voltage from 4600 to 7800 V, the discharge mode is changed from single-pulse APGD with filamentary discharge to two-pulse APGD with filamentary discharge, and the Lissajous figure also converts from a quadrilateral with one step to two steps on the right-hand side.     

Numerical simulation of plasma-assisted combustion of methane-air mixtures in combustion chamber

A two-dimensional mathematical model was developed to investigate the effects of dielectric barrier discharge (DBD) plasma on CH₄-air mixtures combustion at atmospheric pressure. Considering the physical and chemical processes of plasma-assisted combustion (PAC), plasma discharge, heat transfer and turbulent were simultaneously coupled into simulation of PAC. This coupling model consists of DBD kinetic model and methane combustion model. By comparing simulations and the original reference’s results, a high-accuracy of this model was validated. In addition, the effects of PAC actuation parameters on combustion characteristics were studied. Numerical simulations show that with an inlet airflow velocity of 10 ms ^-1, a CH₄-air mixtures’ equivalence ratio of 0.5, an applied voltage of 10 kV, a frequency of 1200 kHz, compared to conventional combustion (CC), the highest flame temperature rises by 32 K; outlet temperature distribution coefficient drops by 2.3%; the maximum net reaction rate of CH₄ and H₂O increase by 11.22% and 12.80% respectively; the maximum CO emission index decreases by 14.61%; the mixing region turbulence mixing time reduces by 89 ms.