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.     

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.     

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.     

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.     

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.     

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.     

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.     

DeNOx Study in Diesel Engine Exhaust Using Barrier DischargeCorona Assisted by V2O5／TiO2 Catalyst

A plasma-assisted catalytic reactor was used to remove nitrogen oxides (NOx) from diesel engine exhaust operated under different load conditions. Initial studies were focused on plasma reactor (a dielectric barrier discharge reactor) treatment of diesel exhaust at various temperatures. The nitric oxide (NO) removal efficiency was lowered when high temperature exhaustwas treated using plasma reactor. Also, NO removal efficiency decreased when 45% load exhaust was treated. Studies were then made with plasma reactor combined with a catalytic reactor consisting of a selective catalytic reduction (SCR) catalyst, V2O5/TiO2. Ammonia was used as a reducing agent for SCR process in a ratio of 1:1 to NOx. The studies were focused on temperatures of the SCR catalytic reactor below 200℃. The plasma-assisted catalytic reactor was operated well to remove NOx under no-load and load conditions. For an energy input of 96 J/1, the NOx removal efficiencies obtained under no-load and load conditions were 90% and 72% respectively at an exhaust temperature of 100℃.     

电子束辐照处理模拟甲苯废气实验研究

以甲苯作为挥发性有机化合物的代表物质,在800keV电子束的辐照下,模拟甲苯废气的气量在0.5—1.2m3/h范围内,研究了甲苯初始质量浓度为1600—4630mg/m3时吸收剂量、甲苯初始浓度和湿度对于甲苯分解效率的影响。实验结果表明,电子束辐照可有效去除甲苯,甲苯初始质量浓度为1600mg/m3,辐照10kGy和40kGy,甲苯去除率分别为46.5%和72.2%;增加湿度也可提高甲苯去除率。用气相色谱-质谱仪(GC-MS)和离子色谱仪(IC)定性研究了辐解产物。甲苯辐解产物比较复杂,主要含有苯甲醛、甲酸等物质。也探讨了电子束辐照处理甲苯气体的主要机理,讨论了O2和.OH对于电子束辐照分解甲苯中的重要作用。     

Conversion of NO with a catalytic packed-bed dielectric barrier discharge reactor

This paper discusses the conversion of nitric oxide (NO) with a low-temperature plasma induced by a catalytic packed-bed dielectric barrier discharge (DBD) reactor.Alumina oxide (Al2O3),glass (SiO2) and zirconium oxide (ZrO2),three different spherical packed materials of the same size,were each present in the DBD reactor.The NO conversion under varying input voltage and specific energy density,and the effects of catalysts (titanium dioxide (TiO2) and manganese oxide (MnOx) coated on Al2O3) on NO conversion were investigated.The experimental results showed that NO conversion was greatly enhanced in the presence of packed materials in the reactor,and the catalytic packed bed of MnOx/Al2O3 showed better performance than that of TiO2/Al2O3.The surface and crystal structures of the materials and catalysts were characterized through scanning electron microscopy analysis.The final products were clearly observed by a Fourier transform infrared spectrometer and provided a better understanding of NO conversion.     

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.     

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%.     

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.     

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.     

Decomposition of dioxin-like components in a DBD reactor combined with Hg/Ar electrodeless ultraviolet

A new combined reactor with Hg/Ar electrodeless ultraviolet(EDUV)activated by DBD for 3,4-dichlorodiphenyl ether abatement is presented.The effect of specific input energy and feeding gas component on 3,4-dichlorodiphenyl ether removal efficiency has been explored.Compared with a single DBD system,this new combined process performed a significant promotion on 3,4-dichlorodiphenyl ether abatement.Experiment results verified that active oxygen clearly contributed to the synergistic activity of DBD-EDUV system.Results of emission spectra showed that UV radiation of 253.7 nm could be detected in the DBD-EDUV system.Further,the products of DBD-EDUV process were analyzed via gas chromatographymass spectrometer(GC-MS)to reveal involved decomposition mechanism.     

Analysis of loss of coolant accident in MTR pool type research reactor

In MTR research reactors, heat removal is, safely performed by forced convection during normal operation and by natural convection after reactor shutdown for residual decay heat removal. However, according to the duration time of operation at full power, it may be required to maintain the forced convection, for a certain period of time after the reactor shutdown. This is among the general requirements for the overall safety engineering features of MTR research reactors to ensure a safe residual heat removal. For instance, in safety analysis of research reactors, initiating events that may challenge the safe removal of residual heat must be identified and analyzed.In the present work, it was assumed a total loss of coolant accident in a typical MTR nuclear research reactor with the objective of examining the core behavior and the occurrence of any fuel damage.For this purpose, the IAEA 10 MW benchmark core, which is a representative of medium power pool type MTR research reactors, was chosen herein in order to investigate the evolution of cladding temperature through the use of a best estimate thermalhydraulic system code RELAP5/mod3.2.     

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.     

严重事故下吸湿性气溶胶的自然去除研究

反应堆发生严重事故时，堆芯释放出的吸湿性气溶胶会在潮湿的安全壳内增大，从而影响其自然去除过程。本文理论推导了吸湿性气溶胶的增大模型并通过多种方法对其进行了验证。模型计算结果表明，气溶胶的增大过程由于受到溶解度的限制而存在临界湿度值，在该临界值以下时气溶胶不发生吸湿，但这未被其他严重事故分析程序所考虑。同时，基于某三代先进压水堆的特定严重事故工况，本文分析了干颗粒半径及湿度对气溶胶的平衡半径和自然去除系数的影响。结果表明:气溶胶的自然去除系数随干颗粒半径的增大将先减小后增加，并在1 μm时达到最小值；相同湿度下，干颗粒半径对气溶胶半径的最大增大比例的影响不大；湿度的增加对不同干颗粒半径气溶胶去除系数的影响不同。      

熔盐堆主回路系统氙的动力学特性研究

基于Mathematica7.0为熔盐堆（MSR）主回路系统建立了一套含流动项及在线去除功能的氙（135Xe）的动态分布数值分析程序，针对2?MW MSR的一种设计方案，分析了不同流量、不同启停堆功率、不同在线去除效率情况下135Xe浓度随时间的动态变化特性。结果表明:相较于静态燃耗模型，流动燃耗模型的135Xe带来的负反应性要低约32.2%；额定流量下主回路系统135Xe浓度分布均匀，只有当主回路系统体积流量小于2.24 cm3·s-1时，流动效应才会对主回路系统内135Xe浓度分布有显著影响；当鼓泡系统的在线去除份额约为0.1%时可以使堆芯135Xe带来的负反应性降低至-38.3 pcm?（1 pcm =10-5），其总的去除效率可以达到86.0%；不同功率水平瞬时停堆工况下，堆芯135Xe浓度单调下降，停堆约50 h后135Xe基本消失，相当于引入+254 pcm反应性，停堆过程无碘坑出现，停堆后再启堆过程不必担心碘坑启动的问题。135Xe去除效率对整个系统135Xe总量有一定影响，在去除份额从0.0001%~20%的变化范围内，135Xe的总活度与静态燃耗模型相比相应增加了0.67%~8.75%。      

Above-ground HTGR design for passive decay heat removal

The design of a small high-temperature gas-cooled reactor (HTGR) for passive decay heat removal which could be located deeply underground was proposed previously. In the present work, analogue design analyses of passive decay heat removal for an above-ground long-life small prismatic HTGR was carried out to obtain the conditions for successful decay heat removal by radiation and conduction inside the reactor building, and by radiation and natural cooling by air at the outer surface of the reactor building. Sensitivity analysis of the peak temperatures of both the core and the reactor building after reactor shutdown was performed by changing the physical characteristics of the reactor regions. Enlarging the reactor building was found to be an effective way to reduce the peak reactor building temperature to within its design limit. By using the obtained condition for design parameters, the appropriate sizes of reactor core and reactor building were evaluated for some reactors. Consequently, criticality and burnup analyses for the proposed reactors were performed to confirm the possibility of designing a long-life core for the core size and reactor power which meet the condition of removing decay heat successfully. Using our design, all the reactors with 20 wt% uranium enrichment could be critical for over nine years.