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.     

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.     

Oxidative Degradation of 4-chlorophenol in Aqueous Induced by Plasma with Submersed Glow Discharge Electrolysis

The oxidative degradation of 4-chlorophenol （4-CP） in aqueous solution induced by plasma with submersed glow discharge has been investigated. The concentration of 4-CP and the reaction intermediates were determined by high performance liquid chromatography （HPLC）. Various influencing factors such as the initial pH, the concentration of 4-CP and the catalytic action of Fe^2＋ were examined. The results indicate that 4-CP is eventually degraded into inorganic ion, dioxide carbon and water. The attack of hydroxyl radicals on the benzene rings of 4-CP in the initial stage of oxidative reactions is presumed to be a key step. They also suggest that the reaction is of a pseudo-first order kinetic reaction and the proposed method is an efficient way for the 4-CP degradation,     

Effect of insulating oil covering electrodes on the characteristics of a dielectric barrier discharge

In this study, the effects of the fluid cooling and electric field line deformation were investigated in a dielectric barrier discharge (DBD) plasma source. The DBD plasma jet is improved by covering the ground electrode and a power electrode with insulating oil. We obtained positive results as insulating oil prevents arc formation, while it improved the supplied power and plasma jet length, and increased radical production. Radical production of this nonthermal plasma jet is studied with polyvinyl alcohol–potassium iodide liquid.     

Degradation and mineralization of ciprofloxacin by gas–liquid discharge non-thermal plasma

A typical quinolones antibiotic ciprofloxacin(CIP) in aqueous solution was degraded by a gas–liquid discharge non-thermal plasma system. The discharge plasma power and the emission intensity of the excited reactive species(RS) generated in the gas phase were detected by the oscilloscope and the optical emission spectroscopy. The effects of various parameters on CIP degradation, i.e. input powers, initial concentrations addition of radical scavengers and p H values were investigated. With the increase of discharge power, the degradation efficiency increased but the energy efficiency significantly reduced. The degradation efficiency also reduced under high concentration of initial CIP conditions due to the competitive reactions between the plasma-induced RS with the degradation intermediates of CIP. Different radical scavengers(isopropanol and CCl_4) on ·OH and H· were added into the reaction system and the oxidation effects of ·OH radicals have been proved with high degradation capacity on CIP.Moreover, the long-term degradation effect on CIP in the plasma-treated aqueous solution proved that the long-lived RS(H_2O_2 and O_3, etc) might play key roles on the stay effect through multiple aqueous reactions leading to production of ·OH. The degradation intermediates were determined by the method of electrospray ionization(+)-mass spectroscopy, and the possible degradation mechanism were presented.     

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%.     

Oxidation of ciprofloxacin by the synergistic effect of DBD plasma and persulfate: reactive species and influencing factors analysis

A synergistic system of water falling film dielectric barrier discharge(DBD) plasma and persulfate(PS) was set up and used for oxidizing ciprofloxacin(CIP) in water. Results of reactive species formation in the DBD-only system as well as the DBD–PS system verified the PS activation in the DBD system. Influencing factors on CIP degradation and the degradation process were also been studied. The obtained results showed that the presence of PS could greatly improve the degradation and mineralizatio...     

Discoloration of Congo Red by Rod-Plate Dielectric Barrier Discharge Processes at Atmospheric Pressure

A dielectric barrier discharge (DBD) reactor with a rod-plate electrode configuration was used for the oxidative decomposition of Congo red dye in an aqueous solution.Plasma was generated in the gas space above the water interface under atmospheric pressure.Discharge characteristics were analyzed by voltage-current waveforms.Effects of applied voltage,initial conductivity,and initial concentration were also analyzed.Congo red discoloration increased with increased applied voltage and decreased conductivity.The initial conductivity significantly influenced the Congo red discoloration.Under the same conditions,the highest discoloration rate was obtained at 25 mg/L.The presence of ferrous ions in the solutions had a substantial positive effect on Fenton dye degradation and flocculation.At an applied voltage of 20 kV,about 100％of dye was degraded after 4 min of Fe2+/DBD treatment.Results showed that adding a certain dosage of hydrogen peroxide to the wastewater could enhance the discoloration rate.Possible pathways of Congo red discoloration by DBD plasma were proposed based on GC/MS,FTIR,and UV-vis spectroscopy analyses.     

Study of Humidity Effect on Benzene Decomposition by the Dielectric Barrier Discharge Nonthermal Plasma Reactor

The humidity effects on the benzene decomposition process were investigated by the dielectric barrier discharge(DBD) plasma reactor.The results showed that the water vapor played an important role in the benzene oxidation process.It was found that there was an optimum humidity value for the benzene removal efficiency,and at around 60% relative humidity(RH),the optimum benzene removal efficiency was achieved.At a SIE of 378 J/L,the removal efficiency was 66% at 0% RH,while the removal efficiency reached 75.3% at 60% RH and dropped to 69% at 80% RH.Furthermore,the addition of water inhibited the formation of ozone and NO_2 remarkably.Both of the concentrations of ozone and NO_2 decreased with increasing of the RH at the same specific input energy.At a SIE of 256 J/L,the concentrations of ozone and NO_2 were 5.4 mg/L and 1791 ppm under dry conditions,whereas they were only 3.4 mg/L and 1119 ppm at 63.5%RH,respectively.Finally,the outlet gas after benzene degradation was qualitatively analyzed by FT-IR and GC-MS to determine possible intermediate byproducts.The results suggested that the byproducts in decomposition of benzene primarily consisted of phenol and substitutions of phenol.Based on these byproducts a benzene degradation mechanism was proposed.     

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.     

Degradation of α-Naphthol by Plasma in Aqueous Solution

1. IntroductionContact glow--discharge electrolysis (CGDE) isa novel type of electrochendcal process in whichplasma is sustained by dc glow discharges between anelectrode and the surface of the electrolyte. The conventional normal electrolysis is evolved into CGDEwhen the applied voltage is sufficiently high in aqueous media. In a full glow discharge, the novel chemical yields of anodic CGDE originate from the primary reaction zones) which consists of the plasmaaround the anode and the li…     

Numerical study of the influence of dielectric tube on propagation of atmospheric pressure plasma jet based on coplanar dielectric barrier discharge

A 2D fluid model was employed to simulate the influence of dielectric on the propagation of atmospheric pressure helium plasma jet based on coplanar dielectric barrier discharge (DBD). The spatio-temporal distributions of electron density, ionization rate, electrical field, spatial charge and the spatial structure were obtained for different dielectric tubes that limit the helium flow. The results show that the change of the relative permittivity of the dielectric tube where the plasma jet travels inside has no influence on the formation of DBD itself, but has great impact on the jet propagation. The velocity of the plasma jet changes drastically when the jet passes from a tube of higher permittivity to one of lower permittivity, resulting in an increase in jet length,ionization rate and electric field, as well as a change in the distribution of space charges and discharge states. The radius of the dielectric tube has a great influence on the ring-shaped or solid bullet structure. These results can well explain the behavior of the plasma jet from the dielectric tube into the ambient air and the hollow bullet in experiments.     

Strengthening decomposition of oxytetracycline in DBD plasma coupling with Fe-Mn oxide-loaded granular activated carbon

A catalytic approach using a synthesized iron and manganese oxide-supported granular activated carbon (Fe-Mn GAC) under a dielectric barrier discharge (DBD) plasma was investigated to enhance the degradation of oxytetracycline (OTC) in water. The prepared Fe-Mn GAC was characterized by x-ray diffraction and scanning electron microscopy, and the results showed that the bimetallic oxides had been successfully spread on the GAC surface. The experimental results showed that the DBD + Fe-Mn GAC exhibited better OTC removal efficiency than the sole DBD and DBD + virgin GAC systems. Increasing the fabricated catalyst and discharge voltage was favorable to the antibiotic elimination and energy yield in the hybrid process. The coupling process could be elucidated by the ozone decomposition after Fe-Mn GAC addition, and highly hydroxyl and superoxide radicals both play significant roles in the decontamination. The main intermediate products were identified by HPLC-MS to study the mechanism in the collaborative system.     

Plasma-catalytic degradation of tetracycline hydrochloride over Mn/γ-Al2O3 catalysts in a dielectric barrier discharge reactor

A coaxial dielectric barrier discharge (DBD) reactor was used for plasma-catalytic degradation of tetracycline hydrochloride over a series ofMn/γ-Al₂O₃ catalysts prepared by the incipient wetness impregnation method. The combination of plasma and theMn/γ-Al₂O₃ catalysts significantly enhanced the degradation efficiency of tetracycline hydrochloride compared to the plasma process alone, with the 10%Mn/γ-Al₂O₃ catalyst exhibiting the best tetracycline hydrochloride degradation efficiency. A maximum degradation efficiency of 99.3% can be achieved after 5 min oxidation and a discharge power of 1.3 W, with only 69.7% by a single plasma process. The highest energy yield of the plasma-catalytic process is 91.7 gkWh⁻¹. Probable reaction mechanisms of the plasma-catalytic removal of tetracycline hydrochloride were also proposed.     

Naphthalene oxidation by different non-thermal electrical discharges at atmospheric pressure

Gaseous naphthalene has been removed by air plasma generated by pulsed corona discharges at 100°C (LSPM) and dielectric barrier discharges (DBD) up to 250 °C (LPGP) in different reactors geometries. Naphthalene has been chosen as one of unburned hydrocarbon present in exhaust gas engine during the cold start of vehicles. The comparison between the different discharge geometries has been possible using the specific input energy (SIE) as relevant parameter for pollutant removal process control considering the differences in the electrical characteristics and the differences of gas flow. The best naphthalene degradation is obtained in the wire-to cylinder (WTC) corona discharge and the stem-to-cylinder DBD with an energy cost β respectively of 10 and 20 J L ^-1. The main by-products issues of the naphthalene oxidation are CO₂ and CO reaching 45% in Multi-Pin-to-Plan corona discharge. We detected polyaromatic hydrocarbons in the gas phase (few ppm) and in the solid phase deposited in the reactors. The introduction of water in the discharges promotes the naphthalene degradation by OH-atom, which has better oxidising power than O-atom in dry air.     

Research on quinoline degradation in drinking water by a large volume strong ionization dielectric barrier discharge reaction system

Quinoline is widely used in the production of drugs as a highly effective insecticide, and its derivatives can also be used to produce dyes. It has a teratogenic carcinogen to wildlife and humans once entering into the aquatic environment. In this study, the degradation mechanism of quinoline in drinking water by a strong ionization dielectric barrier discharge(DBD) lowtemperature plasma with large volume was explored. High concentration of hydroxyl radical(·OH)(0.74 mmol l-1) and ozone(O3)(58.2 mg l-1) produced by strongly ionized discharge DBD system were quantitatively analyzed based on the results of electron spin resonance and O3 measurements. The influencing reaction conditions of input voltages, initial p H value, ·OH inhibitors, initial concentration and inorganic ions on the removal efficiency of quinoline were systematically studied. The obtained results showed that the removal efficiency and TOC removal of quinoline achieved 94.8% and 32.2%, degradation kinetic constant was 0.050 min-1 at 3.8 k V and in a neutral p H(7.2). The proposed pathways of quinoline were suggested based on identified intermediates as hydroxy pyridine, fumaric acid, oxalic acid, and other small molecular acids by high-performance liquid chromatography/tandem mass spectrometry analysis. Moreover, the toxicity analysis on the intermediates demonstrated that its acute toxicity, bioaccumulation factor and mutagenicity were reduced. The overall findings provided theoretical and experimental basis for the application of a high capacity strong ionization DBD water treatment system in the removal of quinoline from drinking water.     

Non-Thermal Equilibrium Atmospheric Pressure Glow-Like Discharge Plasma Jet

Non-thermal equilibrium atmospheric pressure plasma jet (APPJ) is a cold plasma source that promises various innovative applications,and the uniform APPJ is more favored.Glow discharge is one of the most effective methods to obtain the uniform discharge.Compared with the glow dielectric barrier discharge (DBD) in atmospheric pressure,pure helium APPJ shows partial characteristics of both the glow discharge and the streamer.In this paper,considering the influence of the Penning effect,the electrical and optical properties of He APPJ and Ar/NH3 APPJ were researched.A word "Glow-like APPJ" is used to characterize the uniformity of APPJ,and it was obtained that the basic characteristics of the glow-like APPJ are driven by the kHz AC high voltage.The results can provide a support for generating uniform APPJ,and lay a foundation for its applications.     

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.     

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.     

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.