Effect of Water Vapor on Toluene Removal in Catalysis-DBD Plasma Reactors

The experiment was carried out in a cylindrical dielectric barrier discharge(DBD)reactor assisted with a catalyst to decompose toluene under different humidity.In order to explore the synergistic effect on removing toluene in the catalysis-DBD reactor,this paper investigated the decomposition efficiency and the energy consumption in the catalysis-DBD and the non-catalyst DBD reactors under different humidity.The results showed that the catalysis-DBD reactor had a better performance than the non-catalysis one at the humidity ratio of 0.4%,and the removal efficiency of toluene could reach 88.6% in the catalysis-DBD reactor,while it was only 59.9% in the non-catalytic reactor.However,there was no significant difference in the removal efficiency of toluene between the two reactors when the humidities were 1.2% and 2.4%.Additionally,the degradation products were also analyzed in order to gain a better understanding of the mechanism of decomposing toluene in a catalysis-DBD reactor.     

Enhancing toluene removal in a plasma photocatalytic system through a black TiO_2 photocatalyst

An efficient toluene removal in air using a plasma photocatalytic system(PPS) not only needs favorable surface reactions over photocatalysts under the action of plasma,but also requires the photocatalysts to efficiently absorb light emitted from the discharge for driving the photocatalytic reactions. We report here that the PPS constructed by integrating a black titania(B-TiO_2)photocatalyst with a dielectric barrier discharge(DBD) can effectively remove toluene with above 70% CO_2 selectivity and remarkably reduced the concentration of secondary pollutants of ozone and nitrogen oxides at a specific energy input of 1500 J·l~(-1),while exhibiting good stability. Photocatalyst characterizations suggest that the B-TiO_2 provides a high concentration of oxygen vacancies for the surface oxidation of toluene in DBD,and efficiently absorbs ultraviolet–visible light emitted from the discharge to induce plasma photocatalytic oxidation of toluene. The presence of B-TiO_2 in the plasma region also results in a high discharge efficiency,facilitating the generation of large numbers of reactive species and thus the oxidation of toluene towards CO_2. The greatly enhanced performance of the PPS integrated with B-TiO_2 in toluene removal offers a promising approach to efficiently remove refractory volatile organic compounds from air at low temperatures.     

Diagnostics of Argon Inductively Coupled Plasma and Dielectric Barrier Discharge Plasma by Optical Emission Spectroscopy

1. IntroductionArgon plasma has been frequently used for mate-rial processing and film fabrication processes [1l [21 [31.The efficiency of these processes has very close rela-tion with plasma parameters [4][5], such as ion den-sity, electron temperature and ion energy dlstrlbu-tion. Lots of research has been done on the relation-ship between efficiency and availability of materialprocessing and plasma parameters [6][7].Both lCP dlscharge and DBD discharge are newtype plasma systems developed…     

Enhanced removal of ultrafine particles from kerosene combustion using a dielectric barrier discharge reactor packed with porous alumina balls

Ultrafine particles(UFPs) are harmful to human beings, and their effective removal from the environment is an urgent necessity. In this study, a dielectric barrier discharge(DBD) reactor packed with porous alumina(PA) balls driven by a pulse power supply was developed to remove the UFPs(ranging from 20 to 100 nm) from the exhaust gases of kerosene combustion. Five types of DBD reactors were established to evaluate the effect of plasma catalysis on the removal efficiency of UFPs. The influences of gas flow rate, peak voltage and pulse frequency of different reactors on UFPs removal were investigated. It was found that a high total UFP removal of91.4% can be achieved in the DBD reactor entirely packed with PA balls. The results can be attributed to the enhanced charge effect of the UFPs with PA balls in the discharge space. The UFP removals by diffusion deposition and electrostatic attraction were further calculated,indicating that particle charging is vital to achieve high removal efficiency for UFPs.     

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...     

DBD coupled with MnOx/γ-Al2O3 catalysts for the degradation of chlorobenzene

This paper investigates the degradation of chlorobenzene by dielectric barrier discharge(DBD)coupled with MnOx/γ-Al2O3 catalysts.MnOx/γ-Al2O3 catalysts were prepared using the impregnation method and were characterized in detail by N2 adsorption/desorption,x-ray diffraction and x-ray photoelectron spectroscopy.Compared with the single DBD reactor,the coupled reactor has a better performance on the removal rate of chlorobenzene,the selectivity of COx,and the inhibition of ozone production,especially at low discharge voltages.The degradation rate of chlorobenzene and selectivity of COx can reach 96.3%and 53.0%,respectively,at the specific energy density of 1350 J l-1.Moreover,the ozone concentration produced by the discharge is significantly reduced because the MnOx/Al2O3 catalysts contribute to the decomposition of ozone to form oxygen atoms for the oxidation of chlorobenzene.In addition,based on analysis of the byproducts,the decomposition mechanism of chlorobenzene in the coupled reactor is also discussed.     

Investigation on discharge characteristics of a coaxial dielectric barrier discharge reactor driven by AC and ns power sources

A coaxial dielectric barrier discharge(DBD) reactor with double layer dielectric barriers has been developed for exhaust gas treatment and excited either by AC power or nanosecond(ns)pulse to generate atmospheric pressure plasma. The comparative study on the discharge characteristics of the discharge uniformity, power deposition, energy efficiency, and operation temperature between AC and ns pulsed coaxial DBD is carried out in terms of optical and electrical characteristics and operation temperature for optimizing the coaxial DBD reactor performance. The voltages across the air gap and dielectric layer and the conduction and displacement currents are extracted from the applied voltages and measured currents of AC and ns pulsed coaxial DBDs for the calculation of the power depositions and energy efficiencies through an equivalent electrical model. The discharge uniformity and operating temperature of the coaxial DBD reactor are monitored and analyzed by optical images and infrared camera. A heat conduction model is used to calculate the temperature of the internal quartz tube. It is found that the ns pulsed coaxial DBD has a much higher instantaneous power deposition in plasma, a lower total power consumption, and a higher energy efficiency compared with that excited by AC power and is more homogeneous and stable. The temperature of the outside wall of the AC and ns pulse excited coaxial DBD reaches 158 ℃ and 64.3 ℃ after 900 s operation, respectively.The experimental results on the comparison of the discharge characteristics of coaxial DBDs excited by different powers are significant for understanding of the mechanism of DBDs,reducing energy loss, and optimizing the performance of coaxial DBD in industrial applications.     

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.     

Degradation of Dye Wastewater by ns-Pulse DBD Plasma

Two plasma reactors have been developed and used to degrade dye wastewater agents.The configuration of one plasma reactor is a comb-like extendable unit module consisting of 5 electrodes covered with a quartz tube and the other one is an array reactor which is extended from the unit module.The decomposition of wastewater by ns pulse dielectric barrier discharge(DBD) plasma have been carried out by atomizing the dyeing solutions into the reactors.During experiments,the indigo carmine has been treated as the waste agent.The measurements of UV-VIS absorption spectroscopy and the chemical oxygen demand(COD) are carried out to demonstrate the decomposition efect on the wastewater.It shows that the decoloration rate of 99% and the COD degradation rate of 65% are achieved with 15 min treatment in the unit reactor.The efect of electrical parameters on degradation has been studied in detail.Results from the array reactor indicate that it has a better degradation efect than the unit one.It can not only totally remove the chromogenic bond of the indigo carmine solution,but also efectively degrade unsaturated bonds.The decoloration rate reaches 99% after 10 min treatment,the decomposition rate of the unsaturated bond reaches 83% after 60 min treatment,and the COD degradation rate is nearly 74%.     

Degradation of phenol using a combination of granular activated carbon adsorption and bipolar pulse dielectric barrier discharge plasma regeneration

A combined method of granular activated carbon (GAC) adsorption and bipolar pulse dielectric barrier discharge (DBD) plasma regeneration was employed to degrade phenol in water. After being saturated with phenol, the GAC was filled into the DBD reactor driven by bipolar pulse power for regeneration under various operating parameters. The results showed that different peak voltages, air flow rates, and GAC content can affect phenol decomposition and its major degradation intermediates, such as catechol, hydroquinone, and benzoquinone. The higher voltage and air support were conducive to the removal of phenol, and the proper water moisture of the GAC was 20％. The amount of H2O2 on the GAC was quantitatively determined, and its laws of production were similar to phenol elimination. Under the optimized conditions, the elimination of phenol on the GAC was confirmed by Fourier transform infrared spectroscopy,and the total removal of organic carbons achieved 50.4％. Also, a possible degradation mechanism was proposed based on the HPLC analysis. Meanwhile, the regeneration efficiency of the GAC was improved with the discharge treatment time, which attained 88.5％ after 100 min of DBD processing.     

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.     

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.     

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.     

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.     

Influence of electrical parameters on H2O2 generation in DBD non-thermal reactor with water mist

A dielectric barrier discharge (DBD) reactor is introduced to generate H2O2 by non-thermal plasma with a mixture of oxygen and water mist produced by an ultrasonic atomizer.The results of our experiment show that the energy yield and concentration of the generated H2O2 in the pulsed discharge are much higher than that in AC discharge,due to its high energy efficiency and low heating effect.Micron-sized liquid droplets produced by an ultrasonic atomizer in water mist have large specific surface area,which greatly reduces mass transfer resistance between hydroxyl radicals and water liquids,leading to higher energy yield and H2O2 concentration than in our previous research.The influence of applied voltage,discharge frequency,and environmental temperature on the generated H2O2 is discussed in detail from the viewpoint of the DBD mechanism.The H2O2 concentration of 30 mg 1-1,with the energy yield of 2 g kW-1h 1 is obtained by pulsed discharge in our research.     

Discharge Characteristics of Series Surface/Packed-Bed Discharge Reactor Diven by Bipolar Pulsed Power

The discharge characteristics of the series surface/packed-bed discharge(SSPBD)reactor driven by bipolar pulse power were systemically investigated in this study.In order to evaluate the advantages of the SSPBD reactor,it was compared with traditional surface discharge(SD) reactor and packed-bed discharge(PBD) reactor in terms of the discharge voltage,discharge current,and ozone formation.The SSPBD reactor exhibited a faster rising time and lower tail voltage than the SD and PBD reactors.The distribution of the active species generated in different discharge regions of the SSPBD reactor was analyzed by optical emission spectra and ozone analysis.It was found that the packed-bed discharge region(3.5 mg/L),rather than the surface discharge region(1.3 mg/L) in the SSPBD reactor played a more important role in ozone generation.The optical emission spectroscopy analysis indicated that more intense peaks of the active species(e.g.N_2 and OI) in the optical emission spectra were observed in the packed-bed region.     

Development of a dimensionless parameter for characterization of dielectric barrier discharge devices with respect to geometrical features

Non-thermal plasma (NTP) devices produce excited and radical species that have higher energy levels than their ground state and are utilized for various applications.There are various types of NTP devices,with dielectric barrier discharge (DBD) reactors being widely used.These DBD devices vary in geometrical configuration and operating parameters,making a comparison of their performance in terms of discharge power characteristics difficult.Therefore,this study proposes a dimensionless parameter that is related to the geometrical features,and is a function of the discharge power with respect to the frequency,voltage,and capacitance of a DBD.The dimensionless parameter,in the form of a ratio of the discharge energy per cycle to the gap capacitive energy,will be useful for engineers and designers to compare the energy characteristics of devices systematically,and could also be used for scaling up DBD devices.From the results in this experiment and from the literature,different DBD devices are categorized into three separate groups according to different levels of the energy ratio.The larger DBD devices have lower energy ratios due to their lower estimated surface discharge areas and capacitive reactance.Therefore,the devices can be categorized according to the energy ratio due to the effects of the geometrical features of the DBD devices,since it affects the surface discharge area and capacitance of the DBD.The DBD devices are also categorized into three separate groups using the Kriegseis factor,but the categorization is different from that of the energy ratio.     

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.     

Effects of O2 addition on the plasma uniformity and reactivity of Ar DBD excited by ns pulsed and AC power supplies

Dielectric barrier discharges (DBDs) have been widely used in ozone synthesis, materials surface treatment, and plasma medicine for their advantages of uniform discharge and high plasma-chemical reactivity. To improve the reactivity of DBDs, in this work, the O₂ is added into Ar nanosecond (ns) pulsed and AC DBDs. The uniformity and discharge characteristics of Ar ns pulsed and AC DBDs with different O₂ contents are investigated with optical and electrical diagnosis methods. The DBD uniformity is quantitatively analyzed by gray value standard deviation method. The electrical parameters are extracted from voltage and current waveforms separation to characterize the discharge processes and calculate electron density n_e. The optical emission spectroscopy is measured to show the plasma reactivity and calculate the trend of electron temperature T_e with the ratio of two emission lines. It is found that the ns pulsed DBD has a much better uniformity than AC DBD for the fast rising and falling time. With the addition of O₂, the uniformity of ns pulsed DBD gets worse for the space electric field distortion by O₂⁻, which promotes the filamentary formation. While, in AC DBD, the added O₂ can reduce the intensity of filaments, which enhances the discharge uniformity. The ns pulsed DBD has a much higher instantaneous power and energy efficiency than AC DBD. The ratio of Ar emission intensities indicates that the T_e drops quickly with the addition of O₂ both ns pulsed and AC DBDs and the ns pulsed DBD has an obvious higher T_e and n_e than AC DBD. The results are helpful for the realization of the reactive and uniform low temperature plasma sources.     

Preparation of Copper Nanoparticles Using Dielectric Barrier Discharge at Atmospheric Pressure and its Mechanism简

Dielectric barrier discharge （DBD） cold plasma at atmospheric pressure was used for preparation of copper nanoparticles by reduction of copper oxide （CuO）. Power X-ray diffraction （XRD） was used to characterize the structure of the copper oxide samples treated by DBD plasma. Influences of H2 content and the treating time on the reduction of copper oxide by DBD plasma were investigated. The results show that the reduction ratio of copper oxide was increased initially and then decreased with increasing H2 content, and the highest reduction ratio was achieved at 20% H2 content. Moreover, the copper oxide samples were gradually reduced by DBD plasma into copper nanoparticles with the increase in treating time. However, the average reduction rate was decreased as a result of the diffusion of the active hydrogen species. Optical emission spectra （OES） were observed during the reduction of the copper oxide samples by DBD plasma, and the reduction mechanism was explored accordingly. Instead of high-energy electrons, atomic hydrogen （H） radicals, and the heating effect, excited-state hydrogen molecules are suspected to be one kind of important reducing agents. Atmospheric-pressure DBD cold plasma is proved to be an efficient method for preparing copper nanoparticles.