Application of dielectric barrier discharge (DBD) plasma packed with glass and ceramic pellets for SO2 removal at ambient temperature: optimization and modeling using response surface methodology

Air pollution is a major health problem in developing countries and has adverse effects on human health and the environment. Non-thermal plasma is an effective air pollution treatment technology. In this research, the performance of a dielectric barrier discharge (DBD) plasma reactor packed with glass and ceramic pellets was evaluated in the removal of SO₂ as a major air pollutant from air in ambient temperature. The response surface methodology was used to evaluate the effect of three key parameters (concentration of gas, gas flow rate, and voltage) as well as their simultaneous effects and interactions on the SO₂ removal process. Reduced cubic models were derived to predict the SO₂ removal efficiency (RE) and energy yield (EY). Analysis of variance results showed that the packed-bed reactors (PBRs) studied were more energy efficient and had a high SO₂ RE which was at least four times more than that of the non-packed reactor. Moreover, the results showed that the performance of ceramic pellets was better than that of glass pellets in PBRs. This may be due to the porous surface of ceramic pellets which allows the formation of microdischarges in the fine cavities of a porous surface when placed in a plasma discharge zone. The maximum SO₂ RE and EY were obtained at 94% and 0.81 g kWh⁻¹, respectively under the optimal conditions of a concentration of gas of 750 ppm, a gas flow rate of 2 l min⁻¹, and a voltage of 18 kV, which were achieved by the DBD plasma packed with ceramic pellets. Finally, the results of the model's predictions and the experiments showed good agreement.     

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.     

Measurement of the first Townsend's ionization coefficient for atmospheric pressure neon by a dielectric barrier discharge

Fast photography and optical emission spectroscopy are implemented in a 5 mm neon gap dielectric barrier discharge (DBD) at atmospheric pressure with quartz glass used as the dielectric layer. Results show that it starts with a Townsend discharge and ends at a sub-normal glow discharge in neon DBD. Based on the Townsend discharge, the first ionization coefficient of neon is measured. The measurements are consistent with those at low pressure. Optical emission spectroscopy indicates that the spectra are mainly composed of atomic lines of neon, molecular bands and molecular ion bands originating from inevitable gas impurities (mainly nitrogen). Moreover, spectral lines emitted from atomic neon corresponding to the transitions (2p⁵ 3p → 2p⁵ 3s) are predominant. Although the second positive system of N₂(C³Π_u → B³Π_g) is observed, their intensities are too weak compared with neon's spectrum. The molecular nitrogen ion line of 391.4 nm is observed. It reveals that Penning ionization between high energy neon excited states and the inevitable gas impurities plays an important role in the value of the α coefficient.     

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.     

Plasma propagation in single-particle packed dielectric barrier discharges: joint effects of particle shape and discharge gap

In this work, a single Al₂O₃ particle packed dielectric barrier discharge (DBD) reactor with adjustable discharge gap is built, and the influences of the particle shape (ball and column) and the residual gap between the top electrode and particle on the electrical and optical characteristics of plasma are studied. Our research confirms that streamer discharge and surface discharge are the two main discharge patterns in the single-particle packed DBD reactor. The strong electric field distortion at the top of the ball or column caused by the dielectric polarization effect is an important reason for the formation of streamer discharge. The length of streamer discharge is proportional to the size of the residual gap, but the number of discharge times of a single voltage cycle shows an opposite trend. Compared to the column, a smooth spherical surface is more conducive to the formation of large and uniform surface discharges. The surface discharge area and the discharge intensity reach a maximum when the gap is equal to the diameter of the ball. All in all, the results of this study will provide important theoretical support for the establishment of the synergistic characteristics of discharge and catalysis in plasma catalysis.     

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.     

Design of a MT-DBD reactor for H_2S control

This study aimed to discuss the removal of hydrogen sulfide(H_2S)with non-thermal plasma produced by a multilayer tubular dielectric barrier discharge reactor,which is useful in the field of plasma environmental applications.We explored the influence of various factors upon H_2S removal efficiency(η_(H_2S))and energy yield(Ey),such as specific energy density(SED),initial concentration,gas flow velocity and the reactor configuration.The study showed that we can achieveη_(H_2S)of 91%and the best Ey of 3100 mg kWh~(-1)when we set the SED,gas flow velocity,initial H_2S concentration and layers of quartz tubes at 33.2 J 1~(-1),8.0 m s~(-1),30 mg m~(-3)and five layers,correspondingly.The average rate constant for the decomposition of hydrogen sulfide was 0.206 gm~(-3)s~(-1).In addition,we also presented the optimized working conditions,byproduct analysis and decomposition mechanism.     

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.     

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.     

Volume added surface barrier discharge plasma excited by bipolar nanosecond pulse power in atmospheric air: optical emission spectra influenced by gap distance

In this paper, volume barrier discharge with different gap distances is added on the discharge border of high-voltage electrode of annular surface barrier discharge for generating volume added surface barrier discharge (V-SBD) excited by bipolar nanosecond high-voltage pulse power in atmospheric air. The excited V-SBDs consist of surface barrier discharge (d=0 mm) and volume added surface barrier discharges (d=2 mm and 3 mm). The optical emission spectra are recorded for calculating emission intensities of N₂ (C ³Ⅱ_u →B³Π_g ) and N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ ), and simulating rotational and vibrational temperatures. The influences of gap distance of V-SBD on emission intensity and plasma temperature are also investigated and analyzed. The results show that d=0 mm structure can excite the largest emission intensity of N ₂ (C ³ Π_u →B ³Π_g ), while the existence of volume barrier discharge can delay the occurrence of the peak value of the emission intensity ratio of N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ )/N ₂(C³Π_u →B³Π_g ) during the rising period of the applied voltage pulse and weaken it during the end period. The increasing factor of emission intensity is effected by the pulse repetition rate. The d=3 mm structure has the highest threshold voltage while it can maintain more emission intensity of N₂(C³ Π _u →B ³Π_g ) than that of d=2 mm structure. The structure of d=2 mm can maintain more increasing factor than that of the d=3 mm structure with varying pulse repetition rate. Besides, the rotational temperatures of three V-SBD structures are slightly affected when the gap distance and pulse repetition rate vary. The vibrational temperatures have decaying tendencies of all three structures with the increasing pulse repetition rate.     

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.     

A novel double dielectric barrier discharge reactor with high field emission and secondary electron emission for toluene abatement

Dielectric barrier discharge (DBD) has been extensively investigated in the fields of environment and energy, whereas its practical implementation is still limited due to its unsatisfactory energy efficiency. In order to improve the energy efficiency of DBD, a novel double dielectric barrier discharge (NDDBD) reactor with high field emission and secondary electron emission was developed and compared with traditional DDBD (TDDBD) configuration. Firstly, the discharge characteristics of the two DDBD reactors were analyzed. Compared to TDDBD, the NDDBD reactor exhibited much stronger discharge intensity, higher transferred charge, dissipated power and gas temperature due to the effective utilization of cathode field emission and secondary electron emission. Subsequently, toluene abatement performance of the two reactors was evaluated. The toluene decomposition efficiency and mineralization rate of NDDBD were much higher than that of TDDBD, which were 86.44%–100% versus 28.17%–80.48% and 17.16%–43.42% versus 7.17%–16.44% at 2.17–15.12 W and 1.24–4.90 W respectively. NDDBD also exhibited higher energy yield than TDDBD, whereas the overall energy constant ${k}_{{\rm{overall}}}$ of the two reactors were similar. Finally, plausible toluene decomposition pathway in TDDBD and NDDBD was suggested based on organic intermediates that generated from toluene degradation. The finding of this study is expected to provide reference for the design and optimization of DBD reactor for volatile organic compounds control and other applications.     

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.     

A Simplified Numerical Study of the Kr/Cl2 Plasma Chemistry in Dielectric Barrier Discharge

In this paper, the generation of excimers and exciplexe radiation in mixtures of rare gas with halogen by homogeneous dielectric barrier discharge （DBD） is investigated. The typical characteristics of an excilamp based on KrCl exciplexe molecules and the kinetic processes for the formation and the decay of this molecules in the Kr/Cl₂ mixture are studied. The computer model developed is based on the Kr/Cl₂ mixture chemistry, the equivalent electric circuit and the Boltzmann equations. The importance in the kinetic processes of some species such as the metastable state of Krypton （Kr（3P0,2）） and the negative ion of chloride （Cl） is considered. The results illustrate the time variations of charged species （ne,Kr+,Cl,Cl+,Cl+2,Kr+2）, excited atoms and molecules （Kr（3P0,2）, Kr（3P1）, Cl, Cl2）, the excimers （Kr2,KrCl（B）,KrCl（C）,Kr2Cl） and the UV photon concentrations （in 222nm,235nm,258nm and 325nm range）. The effects of chlorine concentration and the total gas pressure in the Kr-Cl₂ discharge on the electric parameters and radiation emissions are investigated.     

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.     

Degradation of Microcystin-LR by Gas-Liquid Interfacial Discharge Plasma

In this study, we report on the degradation of microcystin-LR （MC-LR） by gas- liquid interracial discharge plasma. The influences of operation parameters such as average input voltage, electrode distance and gas flow rate are investigated. Experimental results indicate that the input voltage and gas flow rate have positive influences on MC-LR degradation, while the electrode distance has a negative one. After 6 min discharge with 25 kV average input voltage and 60 L/h air aerati by discharge both in on, the degradation rate of MC-LR achieves 75.3%. distilled water and MC-LR solution are measured H202 and 03 generated Moreover, an emission spectroscopy is used as an indicator of the processes that take place on the gas-liquid boundary and inside plasma. Varied types of radicals （O, .OH, CO, 03, etc.） are proved to be present in the gas phase during gas-liquid interfacial discharge.     

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.     

Analysis of the critical active species for methylene blue decoloration in a dielectric barrier discharge plasma system

In the paper, a hybrid gas–liquid dielectric barrier discharge (DBD) plasma system was set up to treat a methylene blue (MB) solution. The effects of the change of the carrier gas, the gas bubbling rate and different kinds of scavenger addition, including sodium carbonate (Na₂CO₃), para benzoquinone (p-BQ), triethylenediamine and sodium dihydrogen phosphate (NaH₂PO₄), on the MB decoloration were reviewed to clarify the critical active species for the dye decoloration in the DBD plasma system. The obtained results show that higher decoloration of the MB solution could be achieved when O₂ was used as the carrier gas, which could be 100% after 20 min discharge treatment, and the result confirmed the crucial effect of O₃ in the MB decoloration. Based on the experiments of the scavenger addition, it could be concluded that O₂⁻ and ¹O₂ were two other important reactive oxygen species (ROS) for the MB decoloration. The results of the higher chemical oxygen demand removal and faster disappearance of the characteristic peak of the MB from the UV–vis analysis under O₂ bubbling conditions also proved the critical effect of the ROS formed by O₂ on the MB decoloration.     

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.     

Investigation on pulsed discharge mode in SF6-C2H6 mixtures

The non-chain chemical HF(DF)laser is one of the most powerful electrically-driven lasers operating in mid-infrared,in which SF6-C2H6 mixtures are often used as lasering media.Due to the electronegativity of SF6,the discharge in SF6-C2H6 presents a complicated discharge mode.To achieve reproducible pulsed laser output,pulsed discharge in SF6-C2H6 mixtures is investigated for discharge mode using plane electrodes assisted by array pre-ionization spark pins in cathode surface.Firstly,two modes can be distinguished.One mode is called the selfsustained volume discharge(SSVD),which is characterized by spatial uniformity in the discharge gap and pulse to pulse repeatability.On the contrary,another mode includes random arc passages in the discharge gap and therefore cannot conduct lasering.By varying discharge conditions(gap voltage,gas pressure,etc)two discharge modes are observed.Secondly,the holding scope of the SSVD mode is analyzed for the optimal mixture ratio of 20:1,and the boundary tend of the holding scope of SSVD indicates there exists maximum gas pressure and maximum charging voltage for SSVD.Finally,the peak current of SSVD relates positively to charging voltage,while negatively to gas pressure,from which it is drawn that synchronous electron avalanches initiated by the sliding array overlap spatially into SSVD and thus SSVD is essentially an α ionization avalanche.