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.     

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.     

Analysis and Review of Chemical Reactions and Transport Processes in Pulsed Electrical Discharge Plasma Formed Directly in Liquid Water

Electrical discharges formed directly in liquid water include three general cases where (a) streamer-like plasma channels form in, but do not span, the electrode gap, (b) spark discharges produce transient plasma channels that span the electrode gap, and (c) arc discharges form plasma channels with relatively longer life times. Other factors including the input energy (from <1?J/pulse to >1?kJ/pulse) as well as solution properties and the rates of energy delivery affect the nature of the discharge channels. An understanding of the formation of chemical species, including the highly reactive hydroxyl radical and more stable molecular species such as hydrogen and hydrogen peroxide, in such plasma requires determination of temporal and spatial variations of temperature, pressure, plasma volume, and electrical characteristics including current, voltage (electric field), and plasma conductivity. In spark and arc discharges analysis of the physical processes has focused on hydrodynamic and thermal characterization, while only a limited amount of work has connected these physical processes to chemical reactions. On the other hand, the most successful model of the chemical reactions in streamer-like discharges relies on simple assumptions concerning the temperature and pressure in the plasma channels, while analysis of the physical processes is more limited. This paper reviews the literature on the mathematical modeling of electrical discharges in liquid water spanning the range from streamer-like to spark and arc discharges, and compares the properties and processes in these electrical discharges to those in electron beam radiolysis and ultrasound.     

Parameters of an Electric Discharge in Electrolytes and Physicochemical Processes in an Electrolyte Plasma

The parameters of an atmospheric-pressure electric discharge across an active metal electrode immersed in an electrolyte and the electrolyte surface (the thickness of the plasma sheath produced around the active electrode, the distribution of electric potential in the sheath, electrolyte temperature near the sheath boundary and electrode surface) were measured, and the plasma parameters (electric field strength, mean energy and number density of electrons) were determined. It was shown that the plasma of these atmospheric-pressure discharges is nonequilibrium and the discharge in electrolytes is a new type of electric discharge.     

Pulsed Discharge Regeneration of Diesel Particulate Filters

A novel method for the removal of soot from a diesel particulate filter using pulsed electric discharges is presented. High voltage pulses of between 18 and 25 kV of nano to microsecond duration and with pulse energies of typically 100–200 mJ were applied to the filter via a series spark gap. Initial slow erosion of the soot layer proceeds via the formation of microdischarges. Subsequent spark discharges removed the accumulated soot more effectively from a larger filter volume. Average soot removal rates of ～0.1–0.2 g/min were achieved at 50 Hz breakdown frequency by optimizing both electrode geometry and breakdown voltage. On-engine long term testing of the technology showed soot removal by pulsed discharge to be reliable, efficient and uniform; a total of 100 g of soot was deposited and removed over 18 filter regeneration cycles.     

One-Dimensional Modeling on the Asymmetric Features of a Radio-Frequency Atmospheric Helium Glow Discharge Produced Using a Co-Axial-Type Plasma Generator

In this paper, a one-dimensional transient fluid model is used to investigate the asymmetric characteristics of the radio-frequency atmospheric-pressure helium glow discharges produced using a co-axial-type plasma generator. Based on the analysis of the particle and energy balance processes in the discharge region, the modeling results show that the asymmetric features of the time-averaged plasma parameters, e.g., the species number densities, electron energy and the electric field, become significant resulting from the increase in the discrepancy between the surface areas of the inner and outer electrodes. And the influence of the inner electrode radius on the asymmetric features of the discharges becomes more significant compared with the electrode gap spacing for the cases with smaller inner electrode radius. The calculated asymmetric features of the discharges are also validated by the experimental analysis on the discharge images using the visible image processing technique qualitatively.     

Influence of Polarity and Rise Time of Pulse Voltage Waveforms on Diesel Particulate Matter Removal Using an Uneven Dielectric Barrier Discharge Reactor

The influence of polarity and rise time of the pulse voltage on the removal of particulate matter (PM) emitted from a diesel engine was investigated using a dielectric barrier discharge reactor. Four kinds of pulse voltage waveforms (positive, negative, positive–negative and negative–positive) were used. It was found that the energy efficiency for PM removal is just a function of energy injection and that there are no obvious influences on PM removal and energy efficiency within the voltage waveforms except the negative pulse voltage of a peak voltage below 8 kV. A comparison of PM removals using various kinds of pulse voltage waveforms and different types of plasma reactors is given.     

Studies on Oxidants' Generation in a Foaming Column with a Needle to Dielectric Covered Plate Electrode

The generation of oxidative products in the newly investigated foaming system was improved by a discharge between a high voltage multineedle electrode and a dielectric covered plate electrode. A uniformity of the discharge was observed. The presence of alumina dielectric seems to be responsible of the homogenous spatial distribution of the discharge. The absolute power and energy of the discharge was determined. Besides, in larger gap space the foam quality was improved.This way of oxidant's generation, which might be prospective for the treatment of exhaust gas and wastewater, has not been investigated by the other researchers' groups as yet. During the laboratory test 875 ppm of gaseous ozone, 0.5 mg/l of dissolved ozone and 62 mg/l of hydrogen peroxide was obtained at 14 kV of applied voltage and 5 l/min of oxygen gas flow in the present configuration used for the discharge generation. The average yield of gaseous ozone production ranged 55 gO₃/kWh.     

常压辉光放电等离子体转化CH4制C2烃的研究

采用新型的旋转电极辉光放电反应器, 在常温常压下对辉光等离子体作用下的甲烷转化制C₂烃进行了研究. 在氢气共存条件下, 考察了反应器电极的结构、材料, 输入电场峰值电压和反应物流率等参数对甲烷转化率和C₂烃单程收率及其选择性的影响规律, 同时比较了不同反应器的能量效率. 结果表明: 在本实验条件下, 金属铜材料好于不锈钢, 螺旋形结构优于三排圆盘结构. CH₄转化率和C₂烃选择性和收率均随输入电场峰值电压的升高而增大, 随反应物流量的增加而减小. 从CH₄转化率、C₂烃的收率和选择性的指标来评价这些反应器, 采用旋转螺旋状铜电极反应器时最好, 当反应物流量为60 mL/min时, 甲烷最高转化率为77.31%, 对应的C₂烃收率和选择性分别为75.66%和97.88%; 当能量密度为800 kJ/mol时, 能效最高为13.5%.     

丙烯和氧等离子体直接气相合成环氧丙烷

在室温和大气压下,在针板式反应器中,通过脉冲电晕放电等离子体对分子氧和丙烯直接合成环氧丙烷的活化作用,考察了放电电极间距、电晕放电脉冲电压以及电晕放电重复频率参数对丙烯转化率、环氧丙烷产率和其选择性的影响,反应物及各产物通过在线色谱法进行分析.实验结果表明,在室温和大气压下,用脉冲电晕等离子体法可转化丙烯和氧气直接生成环氧丙烷,适当调节上述各参数可提高环氧丙烷的收率.当反应气总流速为200mL/min,极间距为4mm,脉冲放电电压为18kV,放电频率为120Hz时,环氧丙烷的收率、丙烯的转化率及环氧丙烷的选择性分别为5.15%,19.15%和26.89%.     

Optical study of diffuse bi-directional nanosecond pulsed dielectric barrier discharge in nitrogen

In this study, a bi-directional high voltage pulse with 20 ns rising time is employed to generate diffuse glow-like dielectric barrier discharge plasma with very low gas temperature in N2 using needle-plate electrode configuration at atmospheric pressure. Both the diffuse nanosecond pulsed dielectric barrier discharge images and the optical emission spectra of the discharge are recorded successfully under severe electromagnetic interference. The effects of pulse peak voltage, pulse repetition rate, and the concentrations of Ar and O2 on the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π, 0-0), N2 (C3Πu→B3Πg, 0-0, 337.1 nm), and N2+ (B2Σu+→X2Σg+, 0-0, 391.4 nm) are investigated. The effects of the concentrations of Ar and O2 on the discharge diffuse performance are also studied. It is found that the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π, 0-0), N2 (C3Πu→B3Πg, 0-0, 337.1 nm), and N2+ (B2Σu+→X2Σg+, 0-0, 391.4 nm) rise with increasing pulse peak voltage, pulse repetition rate, and the concentration of Ar, but decrease with increasing the concentration of O2. The main physicochemical processes involved are also discussed.     

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.     

Silver Loading on DBD Plasma-Modified Woven PET Surface for Antimicrobial Property Improvement

In this work, the hydrophilic improvement of a woven PET surface was accomplished by a plasma technique. The woven PET surface was plasma-treated by dielectric barrier discharge (DBD) under various operating conditions (electrode gap distance, plasma treatment time, input voltage, and input frequency) and various gaseous environments (air, O₂, N₂, and Ar) in order to improve its hydrophilicity. It was experimentally found that a decrease in electrode gap distance and an increase in input voltage increased the electric field strength, leading to higher hydrophilicity of the PET surface characterized by wickability and contact angle measurements. In comparisons among the studied environmental gases, air gave the highest hydrophilicity, being comparable to O₂, while Ar and N₂ gave lower hydrophilicity of the woven PET surface. The optimum conditions for a maximum hydrophilicity of the PET surface were an electrode gap distance of 4 mm, a plasma treatment time of 10 s, an output voltage of 15 kV, and a frequency of 350 Hz under air environment. After the plasma treatment under the obtained optimum conditions, the woven PET was loaded with Ag particles using a AgNO₃ aqueous solution in order to obtain the antimicrobial property. The plasma-treated woven PET loaded with Ag particles exhibited good antimicrobial activity against both E. coli (gram-negative bacteria) and S. aureus (gram-positive bacteria).     

滑动弧电极放电等离子体作用甲烷制C2烃的工艺

采用刀片式不锈钢电极放电反应器,以Ar气为稀释气,研究了等离子体作用下甲烷转化制C2烃的工艺条件。考察了CH4流量、高频电源输入电压和电极间距等参数对甲烷转化率、C2烃选择性、收率和反应表观能耗的影响。结果表明,增加CH4流量,表观能耗随之降低;当输入电压和电极间距较小时,甲烷转化率随输入电压和电极间距的增大而增大,但输入电压和电极间距过大时,C2烃收率明显下降,积碳严重。在CH4流量14 mL/min、Ar气流量60 mL/min、高频电源输入电压22 V、电流0.44 A、电极间距4 mm的优化条件下,甲烷最高转化率为43.1%,C2烃收率、选择性和表观能耗分别为40.1%、93.2%和2.41 MJ/mol。C2烃中不饱和烃的体积分数可达95%以上。     

Theoretical–Computational Study of Atmospheric DBD Plasma and Its Utility for Nanoscale Biocompatible Plasmonic Coating

In this study, time-dependent, one-dimensional modeling of a surface dielectric barrier discharge (SDBD) device, driven by a sinusoidal voltage of amplitude 1–3 kV at 20 kHz, in argon is described. An SDBD device with two Cu-stripe electrodes, covered by the quartz dielectric and with the discharge gap of 20 × 10⁻³ m, was assumed, and the time-dependent, one-dimensional discharge parameters were simulated versus time across the plasma gap. The plasma device simulated in the given arrangement was constructed and used for biocompatible antibacterial/antimicrobial coating of plasmonic particle aerosol and compared with the coating strategy of the DBD plasma jet. Simulation results showed discharge consists of an electrical breakdown, occurring in each half-cycle of the AC voltage with an electron density of 1.4 × 10¹⁰ cm⁻³ and electric field strength of 4.5 × 10⁵ Vm⁻¹. With SDBD, the surface coating comprises spatially distributed particles of mean size 29 (11) nm, while with argon plasma jet, the nanoparticles are aggregated in clusters that are three times larger in size. Both coatings are crystalline and exhibit plasmonic features in the visible spectral region. It is expected that the particle aerosols are collected under the ionic wind, induced by the plasma electric fields, and it is assumed that this follows the dominant charging mechanisms of ions diffusion. The cold plasma strategy is appealing in a sense; it opens new venues at the nanoscale to deal with biomedical and surgical devices in a flexible processing environment.     

Calculation of parameters of combined electrical discharges—I Model of constant equivalent gap voltage

The parameters of combined discharges, which represent the superposition on a burning d.c. arc of an impulse discharge, were studied. Simple relationships based on approximating a gap voltage with a constant equivalent value were derived, which enable the calculation of the peak current, peak current time, current pulse duration, energy released in the gap, and current pulse shape from the electrical parameters of the discharge circuit.     

Electrical Features of Radio-frequency,Atmospheric-pressure,Bare-metallic-electrode Glow Discharges

Radio-frequency (RF), atmospheric-pressure glow discharge (APGD) plasmas with bare metallic electrodes have promising prospects in the fields of plasma-aided etching, deposition, disinfection and sterilization, etc. In this paper, an induced gas discharge approach is proposed for obtaining the RF, atmospheric-pressure, γ-mode, glow discharges with pure nitrogen or air as the primary plasma-working gas using bare metallic electrodes. The discharge characteristics, including the discharge mode, the breakdown voltage and discharge voltage for sustaining α mode and/or γ mode discharges, of the RF APGD plasmas of helium, argon, nitrogen, air or their mixtures using a planar-type plasma generator are presented in this study. The uniformity (no filaments) of the discharges is confirmed by the images taken by an iCCD with a short exposure time (10 ns). The effects of different gap spacings and electrode materials on the discharge characteristics, the variations of the sheath thickness and the electron number density are also studied in this paper.     

Selective Synthesis of 2D Mesoporous CuO Agglomerates by Pulsed Spark Discharge in Water

Metal oxide nanomaterials, including copper oxide, have attracted great attention due to their unique physical and chemical properties that are dependent on particle size and morphology. In this study, we propose an alternative technique for the synthesis of 2D mesoporous CuO agglomerates that is both efficient and ecological. This technique is based on the use of pulsed spark discharges between copper electrodes immersed in deionized water. Detailed TEM analyses show that the synthesized CuO nanostructures are composed of elementary nanocrystals with sizes in the order of a few nanometers. Assessments of the effects of applied voltage (5 and 20 kV) and discharge pulse width (100 and 500 ns) demonstrate that the latter parameter influences the size and density of nanocrystals in a nanostructure. Moreover, voltage and pulse width may both be used to finely control the direct optical band gap energy of CuO nanostructures between 3.0 and 3.4 eV. The efficient and ecological technique developed in this study produces 2D mesoporous CuO agglomerates that can be readily used in other processes.

     

A High-Efficiency Reactor for the Pulsed Plasma Conversion of Methane

The authors recently developed a high-frequency pulsed plasma process for methane conversion to acetylene and hydrogen using a co-axial cylindrical (CAC) type of reactor. The energy efficiency represented by methane conversion rate per unit input energy has been improved so that such a pulsed plasma has potential for commercial acetylene production. A pulsed plasma consists of a pulsed corona discharge and a pulsed spark discharge. Most of energy is injected over the duration of the pulsed spark discharge. Methane conversion using this kind of pulsed plasma is a kind of pyrolysis enhanced by the pulsed spark discharge. In this study, a point-to-point (PTP) type of reactor that can produce a discharge channel over the duration of a pulse discharge was used for the pulsed plasma conversion of methane. The energy efficiency and carbon formation on electrodes have been improved. The influences of pulse frequency and pulse voltage on methane conversion rate and product selectivity were investigated. The features of methane conversion using PTP and CAC reactors were discussed.     

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.