Low Cost Compact Nanosecond Pulsed Plasma System for Environmental and Biomedical Applications

Nanosecond pulsed non-thermal atmospheric-pressure plasmas are promising for numerous applications including air and water purification, ozone synthesis, surface sterilization, material processing, and biomedical care. However, the high cost of the nanosecond pulsed power sources has hindered adaptation of the plasma-based technologies for clinical and industrial use. This paper presents a low cost (<100US$) nanosecond pulsed plasma system that consists of a Cockcroft–Walton high voltage charging circuit, a compact nanosecond pulse generator using a spark gap as switch, and a plasma reactor. The nanosecond pulse power source requires only a 12 V DC input, hence is battery operable. Through the optimization of the experimental parameters, pulses with a peak voltage >10 kV, a 3 ns rise time (10 to 90 %), and a 10 ns pulse duration (full width at half maximum) at a pulse repetition rate of up to 500 Hz were achieved in the present study. It has been successfully tested to power three different plasma reactors to form pulsed corona discharges, dielectric barrier discharges, and sliding discharges. The energy efficiency of such a nanosecond pulsed sliding discharge system was assessed in the context of ozone synthesis using air or oxygen as the feed gas, and was found comparable to a previously reported non-thermal plasma system that used commercial high voltage pulsed power sources. This study demonstrated that this low-cost nanosecond pulsed power source can prove to be an energy efficient and simple supply to drive various non-thermal atmospheric-pressure plasma reactors for environmental, medical and other applications.     

Design and Operating Characteristics of a Simple and Reliable DBD Reactor for Use with Atmospheric Air

The paper reports on the construction and operating characteristics of a planar dielectric barrier discharge (DBD) plasma generator. The generator was powered from a commercial frequency inverter at 400 Hz through a high voltage transformer. It could be operated up to a specific energy density (power per gas flow) of 20 Wh/m³. The corresponding power density was about 0.5 W per cubic centimeter of discharge volume. Special emphasis was given to a simple and reliable construction, which was easy to assemble and is based on a new, nonexpensive barrier material with excellent electrical, mechanical, and thermal properties. The modular reactor design allows simple plasma power scale-up. The reactor works with undried ambient air without additional cooling. In the range up to 10 Wh/m³ the ozone generation from ambient air was directly proportional to the energy density at a rate of 60 g O₃ per kWh or 30 ppm/Wh/m³. Thus the generator can serve as an effective source for chemically active radicals in plasma gas cleaning applications.     

非平衡等离子体放电模式及反应器结构对氨气分解制氢的影响

在常压下研究了不同等离子体放电模式及反应器结构对氨分解制氢反应的影响.实验中调节反应器结构分别产生了介质阻挡放电和交流弧放电两种放电模式.通过对两种放电模式的放电图像、电压-电流波形和氨分解过程中等离子体区活性物种的发射光谱(OES)研究发现,与介质阻挡放电相比,交流弧放电为局部强放电,具有更高的电源效率和电子密度.因此,在介质阻挡放电中氨气分子大部分通过生成电子激发态物种NH3*,再与载能电子碰撞断裂N―H键进行氨分解反应;而在交流弧放电中载能电子具有更高的平均电子能量,可直接断裂氨气分子的N―H键生成NH2和NH等高活性物种,促进氨分解反应的进行.结果表明,交流弧放电的氨分解效果要明显优于介质阻挡放电.在交流弧放电模式下不同类型反应器对氨气分解转化率由高到低的顺序为:管-管管-板针-板板-板.在输入功率为30 W,气隙间距为6 mm时,管-管交流弧放电的氨气转化率达到60%左右,而板-板介质阻挡放电的氨气转化率仅为4%.     

Uneven Dielectric Barrier Discharge Reactors for Diesel Particulate Matter Removal

Uneven dielectric barrier discharge (DBD) reactors driven by positive–negative pulse plasma discharges were investigated for particulate matter (PM) removal from a diesel engine. Two kinds of uneven alumina plates and three kinds of uneven stainless steel plates were used to assemble six kinds of uneven DBD reactors of discharge gaps 0.4–1.0 mm. The experimental results show that PM from diesel engines can be removed using the uneven DBD reactors. The maximum PM removal was 67% at 300 W energy injections using the DBD reactor of 0.4 mm gap distance. PM removal increased with decreasing gap distance. The energy efficiency using the uneven DBD reactor of a shorter gap distance was higher than that using the uneven DBD reactor of a longer gap distance as the uneven DBD reactor of a shorter gap distance has a higher PM deposition rate. The energy efficiency was typically in a range of 3–10.6 g/kWh at an energy density of 2–16 J/L. A comparison of this study with reports given by other research groups is given.     

Improvement of PBO fiber surface and PBO/PPESK composite interface properties with air DBD plasma treatment

The interface of fibrous composites is a key factor to the whole properties of the composites. In this study, the effects of air dielectric barrier discharge (DBD) plasma discharge power density on surface properties of poly(p‐phenylene benzobisoxazole) (PBO) fiber and the interfacial adhesion of PBO fiber reinforced poly(phthalazinone ether sulfone ketone) (PPESK) composite were investigated by several characterization methods, including XPS, SEM, signal fiber tensile strength, interlaminar shear strength, and water absorption. After the air DBD plasma treatment at a power density of 41.4 W/cm³, XPS analysis showed that some polar functional groups were introduced on the PBO fiber surface, especially the emergence of a new oxygen‐containing group (?O–C = O group). SEM observations revealed that the air DBD plasma treatment had a great influence on surface morphologies of the PBO fiber, while the signal fiber tensile strength results showed only a small decline of 5.9% for the plasma‐treated fiber. Meanwhile, interlaminar shear strength value of PBO/PPESK composite was increased to 44.71 MPa by 34.5% and water absorption of the composite decreased from 0.46% for the untreated specimen to 0.27%. The results showed that the air DBD plasma treatment can effectively improve the properties of the PBO fiber surface and the PBO/PPESK composite interface. Results obtained from the above analyses also showed that both the fiber surface and the composite interface performance would be reduced when an undue plasma discharge power density was applied. Copyright © 2011 John Wiley & Sons, Ltd.     

Conversion of Methane and Carbon Dioxide in a DBD Reactor: Influence of Oxygen

A continuous plug flow reactor supported by a dielectric barrier discharge (DBD) is used to study the conversion of methane, carbon dioxide, and oxygen at different compositions. The three studied gases were diluted with helium to 3 % with an overall flow rate of 200 sccm. The 13.56 MHz plasma was ignited at atmospheric pressure. The product stream and the inlet flow were analyzed by a FTIR spectrometer equipped with a White-cell and by a quadrupole mass spectrometer. The DBD reactor generates hydrogen, carbon monoxide, ethane, ethene, acetylene, formaldehyde, and methanol. Additional oxygen in the feed has positive effects on the yield of methanol, formaldehyde and carbon monoxide and reduces the total consumed energy. The hydrogen yield reaches its maximum at medium amounts of oxygen in the inlet flow. The conversion of methane increases to a limiting value of about 35 %. Methane rich feeds increase the yield of hydrogen, ethane and methanol. On the other hand, additional oxygen has a negative influence on the produced amount of C2 hydrocarbons. The conversion of methane and carbon dioxide as well as the yield of synthesis gas components and C2 hydrocarbons increases by changing the plasma power to higher values.     

Investigation of the Atmospheric Helium Dielectric Barrier Discharge Driven by a Realistic Distorted-Sinusoidal Voltage Power Source

The non-equilibrium atmospheric-pressure parallel-plate helium dielectric barrier discharge (DBD) driven by a realistic 20 kHz distorted-sinusoidal voltage waveform has been investigated by means of simulations and experiments. A self-consistent one-dimensional fluid modeling code considering the non-local electron energy balance was applied to simulate the helium DBD. The effect of selecting plasma chemistry was investigated by comparing simulations with experiments. The results show that the simulations, which include more excited helium, metastable helium and electron–ion-related reaction channels, can faithfully reproduce the measured discharged temporal current quantitatively. Based on the simulated discharge properties, we have found that there is complicated mode transition of discharges from the long Townsend-like to the “dark current”-like, then to the short primary Townsend-like and the short secondary Townsend-like for the helium DBD that is driven by a realistic distorted-sinusoidal voltage power source. Discharge properties in different periods of discharge are discussed in detail in the paper.     

Surface Functionalization at Atmospheric Pressure by DBD-Based Pulsed Plasma Polymerization

Dielectric barrier discharge (DBD)-based plasma deposition at atmospheric pressure, using glycidyl methacrylate (GMA, methacrylic acid-[2,3-epoxy-propyl ester]) as a prototype precursor was investigated in order to evaluate the applicability of dielectric barrier discharges to obtain plasma polymers with a high degree of structural retention of the starting precursor. Using pulsed excitation of the discharge, up to about 90% of the epoxy groups of GMA can be retained in plasma polymers obtainableat deposition rates in the order of 3–5nm/s. Preliminary investigations of the mechanism of film formation under pulsed plasma conditions indicate that the reaction of intact monomer molecules withsurface radicals generated during the pulses play a prominent role.     

Removal of Carbon Disulfide from Gas Streams Using Dielectric Barrier Discharge Plasma Coupled with MnO2 Catalysis System

The removal of gaseous carbon disulfide (CS₂) via dielectric barrier discharge (DBD) combined with MnO₂ catalysis has been investigated. CS₂ removal and energy yield (EY) had been examined as a function of catalyzer position in DBD reactor, initial CS₂ concentration, input power, and gas residence time. The results showed that DBD combined with MnO₂ catalyst can improve the CS₂ energy and removal efficiency, and MnO₂ catalyst placed in afterglow area can enhance the CS₂ removal efficiency by about 10 % as compared with DBD treatment only. When increasing initial CS₂ concentration and flow rate, a higher EY is obtained. The possible CS₂ removal pathways by DBD combined with MnO₂ were proposed based on the product identification by FT-IR.     

Elimination of Carbon Monoxide in the Gas Streams by Dielectric Barrier Discharge Systems with Mn Catalyst

Elimination of CO in air stream using the plasma catalytic reactors was investigated. Two plasma catalytic systems were evaluated in this study, one consisting of a catalyst-bed packed in plasma zone of a dielectric barrier discharge (DBD) reactor directly (CID reactor), and the other (CAD reactor) consisting of a catalyst-bed after a DBD reactor. The examined operating parameters in this study included applied voltage, discharge power, the lengths of plasma zone and catalyst-bed, and inlet CO concentration. It was found that the glass packed DBD reactor without catalyst cannot eliminate CO in air stream effectively. When MnO_x catalyst applied to DBD reactors, the removal of 1000 ppm CO can achieve to 97% by both type reactors. Under constant energy input condition, the CO removal of a CID reactor increased with the decrease of the initial CO concentration and the increase of the length of catalyst beds. In addition, the operating energy consumption of CID system was lower than that of CAD system.     

Deposition Process Based on Organosilicon Precursors in Dielectric Barrier Discharges at Atmospheric Pressure—A Comparison

Dielectric barrier discharges (DBD) at atmospheric pressure are presented as a tool to create organosilicon deposits on technical planar aluminium substrates (up to 15 × 8 cm²) by admixing small amounts of hexamethyldisiloxane (HMDSO) and tetraethoxysilane (TEOS) to the carrier gas of the discharges. Using barrier materials of different specific capacities (2.6 × 10⁴ and 3.2 pF/cm²) in two electrode arrangements operated at less than 1 W, the influence of the filament properties on the deposition is studied. In comparison to these arrangements, a third electrode setup with a barrier of the specific capacity of 2.9 pF/cm² is operated at approximately 50 W to study the influence of the specific energy of the plasma (energy per molecule) on the deposition process. The plasma chemical process was studied qualitatively by Gas Chromatography, and properties of the plasma-treated substrates were examined by means of X-ray Photoelectron Spectroscopy (XPS), Fourier Transform Infrared (FTIR) spectroscopy, as well as visually.     

Diagnostics of Plasma Behavior and TiO<Subscript>2</Subscript> Properties Based on DBD/TiO<Subscript>2</Subscript> Hybrid System

Plasma catalysis is gaining increasing interest in environmental and energy applications, such as the destruction of gas pollutants and hydrocarbon conversion. In order to further improve the application of plasma catalysis, it is crucial to understand the fundamental mechanisms, especially the mutual interaction between plasma and catalyst. In this paper, a parallel-plate dielectric barrier discharge (DBD) reactor is developed to investigate the plasma behavior and TiO₂ properties in the plasma/catalytic hybrid system. The introduction of TiO₂ thin film coated on the dielectric improves the discharge intensity, which significantly contributes to the enhancement of reactive species and charges. The energy efficiency of generating ozone in DBD/TiO₂ system has been approximately raised by 38% compared to pure DBD when the applied voltage reaches 13 kV. It is fortunately found that the discharge does not change the crystal structure of the TiO₂, but the band gap increases from 3.13 to 3.39 eV, which has been proved to enhance the oxidizability of TiO₂ in the degradation of methyl orange experiment under UV light. The FTIR and XPS spectra also demonstrate that N element is doped into the structure of TiO₂. These results successfully illustrate the plasma behavior and catalyst properties in plasma/catalysis hybrid system and provide reference for the optimization of the plasma catalysis process.     

Air Atmospheric Dielectric Barrier Discharge Plasma Induced Germination and Growth Enhancement of Wheat Seed

Air atmospheric dielectric barrier discharge plasma (DBD) was attempted to pretreat wheat seed to improve its germination and growth in this study. The effects of the DBD plasma treatment on the wheat seed germination, seedling growth, osmotic-adjustment products, lipid peroxidation level, and antioxidant enzymes activity were investigated. The experimental results showed that the DBD plasma treatment with an appropriate time scale could promote the wheat seed germination and seedling growth. The germination potential, germination rate, germination index, and vigor index increased by 26.7, 9.1, 16.9, and 46.9% after 7 min’s DBD plasma treatment, respectively; the root length, shoot length, fresh weight, and dry weight of the seedlings also increased after the DBD plasma treatment. The osmotic-adjustment products, proline and soluble sugar contents, in the wheat seedlings were significantly enhanced after the DBD plasma treatment with an appropriate time scale, while the malondialdehyde content decreased. Moreover, the activities of superoxide dismutase and peroxidase also increased after the DBD plasma treatment. The DBD plasma treatment led to etching effect on the wheat seed coat, resulting in the improvement of its water absorption capacity.     

Preparation and Application of Ca0.8 Sr0.2 TiO3 for Plasma Activation of CO2

Despite a large interest in plasma-assisted catalytic technology (PACT), very little has been reported about the catalytic effects of different dielectric barriers on a dielectric barrier discharge (DBD) reaction. In the present study, Ca_0.8Sr_0.2TiO₃, that possesses a high permittivity, was prepared by liquid phase sintering and used as a dielectric barrier in a DBD reactor to break CO₂. The mechanical and dielectric properties of Ca_0.8Sr_0.2TiO₃ were greatly enhanced by adding 0.5 wt.% Li₂Si₂O₅. A DBD plasma was successfully generated by using this Ca_0.8Sr_0.2TiO₃ as a dielectric barrier and 18.8% CO₂ conversion was achieved with the residence time of 0.17 s at the frequency of 8 kHz, which was much higher than with those using an alumina or a silica glass barrier. It was found that the plasma power increased with the increasing of the permittivity, and finally very dense and strong microdischarges were initiated to decompose CO₂.     

Enhancement of Germination and Seedling Growth of Wheat Seed Using Dielectric Barrier Discharge Plasma with Various Gas Sources

The influences of non-thermal discharge plasma treatment on wheat seed germination and seedling growth were investigated using a dielectric barrier discharge (DBD) plasma system at atmospheric pressure and room temperature. DBD plasma with various gas sources (oxygen, air, argon, and nitrogen) was employed in this study. Germination characteristics, seedling growth parameters, surface changes of the seed coat, permeability, and soluble protein of the seedlings were measured after the DBD plasma treatments. The experimental results showed that moderate-intensity DBD plasma had active impacts on wheat seed germination and seedling growth. Germination potential significantly increased by 24.0, 28.0, and 35.5% after 4 min of the air plasma, nitrogen plasma, and argon plasma treatments, respectively, compared with the control; and the shoot and root length also increased; however, no enhancement was observed after the oxygen plasma treatment. Scanning electron microscope analysis showed that etching effects on the seed coat occurred after the air plasma, nitrogen plasma, and argon plasma treatments, which affected the hygroscopicity and permeability of the wheat seed. In addition, moderate-intensity DBD plasma could also activate several physiological reactions in wheat seed, resulting in the increase of soluble protein production in wheat seedlings.     

Numerical Investigation of Effect of Driving Voltage Pulse on Low Pressure 90%Ar–10%Cl<Subscript>2</Subscript> Dielectric Barrier Discharge

An one-dimensional fluid model is used to study the physico-chemical properties of a 90%Ar–10%Cl₂ plasma produced in dielectric barrier discharges under different driving voltages. The spatio-temporal characteristics of the discharge are obtained by applying a sinusoidal voltage with different amplitudes and frequencies from 350 to 1200 V and 10 to 19 kHz, respectively. As the voltage amplitude increases the plasma electronegativity and plasma radiations are increased and their radiations move toward the cathode vicinity. With decreasing frequency, the plasma radiations move toward the anode vicinity and the plasma electronegativity and its radiations are enhanced. At low voltage amplitudes, plasma most radiates VUV photons while UV radiations take place at higher voltage amplitudes.     

Nitric Oxide Conversion and Ozone Synthesis in a Shielded Sliding Discharge Reactor with Positive and Negative Streamers

Positive and negative streamer discharges in atmospheric pressure air were generated in a shielded sliding discharge reactor at operating voltages as low as 5 kV for a gap length of 1.6 cm. In this reactor, electrodes are placed on top of a dielectric layer and one of the electrodes, generally the one on ground potential, is connected to a conductive layer on the opposite side of the dielectric. The energy per pulse, at the same applied voltage, was more than a factor of seven higher than that of pulsed corona discharges, and more than a factor of two higher than that of sliding discharges without a shield. It is explained on the basis of enhanced electric fields, particularly at the plasma emitting electrode. Specific input energy required for 50 % removal from ~1,000 ppm initial NO could be reduced to ~18 eV/molecule when ozone in the exhaust of negative streamers was utilized. For sliding discharges and pulsed corona discharges this value was ~25 eV/molecule and it was 35 eV/molecule for positive shielded sliding discharges. Also, the ozone energy yield from dry air was up to ~130 g/kW h and highest for negative streamer discharges in shielded sliding discharge reactors. The high energy density in negative streamer discharges in the shielded discharge reactor at the relatively low applied voltages might not only allow expansion of basic studies on negative streamers, but also open the path to industrial applications, which have so far been focused on positive streamer discharges.     

Wet Conversion of Methane and Carbon Dioxide in a DBD Reactor

The influence of water on the plasma assisted conversion of methane and carbon dioxide in a dielectric barrier discharge (DBD) plug flow reactor was studied. The plasma at atmospheric pressure was ignited by a power supply at a frequency of 13.56?MHz. Product formation was studied at a power range between 35 and 70?W. The concentrations of the three gases were altered and diluted with helium to 3?%. FTIR spectroscopy and mass spectroscopy were applied to analyze the inlet and the product streams. The main product of this process are hydrogen, carbon monoxide and ethane. Ethene, ethine, methanol and formaldehyde are generated beside the main products in this DBD in lower concentrations. The conversion of methane, the ratio of the synthesis gas components (n(H₂):n(CO)), and the yield of oxygenated hydrocarbons and hydrogen increases by adding water. The total consumed energy reaches lower values for small amounts of water. Additional water does not influence the generated amount of C2 hydrocarbons and of CO, but decreases the carbon dioxide conversion.     

Increasing the Hydrophobicity of a PP Film Using a Helium/CF<Subscript>4</Subscript> DBD Treatment at Atmospheric Pressure

Plasma surface modification is widely used to tailor the surface properties of polymeric materials. Most treatments are performed using low pressure plasma systems, but recently, atmospheric dielectric barrier discharges (DBDs) have appeared as interesting alternatives. Therefore, in this paper, an atmospheric He + CF₄ DBD is used to increase the hydrophobicity of a polypropylene (PP) film. The surface characterization of the PP film is performed using contact angle measurements, X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM). Results show that the hydrophobic properties of the polymer films are greatly enhanced after plasma treatment as evidenced by an increased contact angle. The incorporation of fluorine on the surface is significant (45 at%), demonstrating the ability of the used DBD set-up to generate fluorine-containing functional groups on the PP surface.     

Influence of Duty Cycle on Ozone Generation and Discharge Using Volume Dielectric Barrier Discharge

The influence of duty cycle on ozone generation and discharge characteristics was investigated experimentally using volume dielectric barrier discharge in both synthetic air and pure oxygen at atmospheric pressure. The discharge was driven by an amplitude-modulated AC high voltage–power supply producing T_ON (a single AC cycle) and T_OFF periods with a widely variable duty cycle. The experimental results show that the energy delivered to the discharge during each AC cycle remains roughly constant and is independent of feed gas, duty cycle and T_OFF. Both average discharge power and ozone concentration show an initial linear increase with duty cycle, and deviate gradually from linearity owing to an increase in gas temperature at higher duty cycles. Nevertheless, ozone yield remains nearly constant (45.7 ± 3.5 g/kWh in synthetic air and 94.7 ± 3.1 g/kWh in pure oxygen) over a wide range of applied duty cycles (0.02–1). This property can be conveniently employed to develop a unique ozone generator with a widely adjustable ozone concentration and simultaneously a constant ozone yield. Additionally, the discharges in synthetic air and pure oxygen have similar electrical characteristics; however, there are observable differences in apparent luminosity, which is weak and white-toned for synthetic air discharge, and bright and blue-toned for pure oxygen discharge.