一种新型大气压毛细管介质阻挡放电冷等离子体射流技术

介绍一种结构设计简单、操作运行方便的新型毫米量级大气压冷等离子体射流发生技术.这种射流可以在大气压条件下，利用多种工作气体(如Ar,He,N₂)，通过毛细管介质阻挡放电(DBD)的方式实现.使用频率为33kHz，峰值电压为1—12kV的双向脉冲电源，利用Ar,He,N₂等工作气体，在毛细管内形成了稳定的冷等离子体射流.放电区域的光辐射空间分布利用商用CCD摄像机记录，从中研究放电形态和空间分布，观察到了在DBD区域的流动气体放电和在毛细管出口处形成的等离子体射流 关键词： 冷等离子体射流 毛细管介质阻挡放电 射流射程 射流激发温度     

Changes in Properties of Dielectric Barrier Discharge Plasma Jets for Different Gases and for Insulating and Conducting Transfer Plates

Dielectric barrier discharge (DBD) plasma jets have been studied extensively in recent years because of its wide range of applications. DBD plasmas can be produced using many different gases and can be applied to a broad variety of surfaces and substrates. This work provides comparisons of DBD plasmas generated using argon (Ar), helium (He), and nitrogen (N₂), as well as their mixtures with water vapor in order to know how some plasma properties are affected by the use of different gases. All plasmas were studied in two different conditions: using a transfer plate made of a conductive material and using a transfer plate made of an insulating one. It was observed that the process of Penning ionization of nitrogen molecules by direct collisions with metastable atoms and molecules is evident and significant only in plasmas that use He as the working gas, which means that He atoms in metastable states have greater ability to transfer energy to molecules of nitrogen in the plasma. The collisions of metastable He with N₂ molecules determine the vibrational temperature (T _vib) values in He plasmas, while in Ar and N₂ plasmas, the T _vib values are determined mainly by collisions of electrons with N₂ molecules. It was noticed that the use of an insulating or a conducting transfer plate as the sample holder affects the results of adhesion between poly(dimethylsiloxane) samples, and it is mainly due to the differences in the plasma power, with a higher plasma power leading to better adhesion.     

Fabricating a reactive surface on the fibroin film by a room-temperature plasma jet array for biomolecule immobilization

A simple dielectric barrier discharge(DBD) jet array was designed with a liquid electrode and helium gas.The characteristics of the jet array discharge and the preliminary polymerization with acrylic acid(AA) monomer were presented.The plasma reactor can produce a cold jet array with a gas temperature lower than 315 K,using an applied discharge power between 6 W and 30 W(V dis × I dis).A silk fibroin film(SFF) was modified using the jet array and AA monomer,and the treated SFF samples were characterized by atomic force microscopy(AFM),scanning electron microscopy(SEM),Fourier transform infrared spectroscopy(FTIR),and contact angle(CA).The deposition rate of the poly acrylic acid(PAA) was able to reach 300 nm/min,and the surface roughness and energy increased with the AA flow rate.The FTIR results indicate that the modified SFF had more carboxyl groups(-COOH) than the original SFF.This latter characteristic allowed the modified SFF to immobilize more quantities of antimicrobial peptide(AP,LL-37) which inhibited the Escherichia coli(E.Coli) effectively.     

Mineralization of flexible mesoporous TiO2 photoanodes using two low‐temperature dielectric barrier discharges in ambient air

Two types of dielectric barrier discharges (DBDs), volume DBD (called Industrial Corona) and coplanar DBD, were used for low temperature (70 °C) atmospheric pressure plasma mineralization of mesoporous methyl‐silica/titanium dioxide nanocomposite photoanodes. The photoanodes with a thickness of approx. 300 nm were inkjet‐printed on flexible polyethylene terephthalate (PET) foils. Plasma treatments of both DBDs led to changes in the chemical stoichiometry and morphology of the mesoporous photoanodes, resulting in a significant increase of the work function from approx. 4.0 to 4.3 eV and 4.8 eV, after plasma mineralization with volume DBD and coplanar DBD, respectively. We also studied the effect of plasma mineralization on the photoelectrochemical properties of the flexible mesoporous TiO₂ photoanodes. Plasma mineralization with volume DBD and coplanar DBD showed different effects on the generated photocurrent in the photoanodes. Although the plasma mineralization with volume DBD showed only a minor effect on the photocurrent, plasma mineralization with coplanar DBD led to significantly higher photocurrents. We found that the enhancement of the photoelectrochemical properties was related to the homogeneity of the plasma‐treated surfaces—arising from different spatial properties of the plasma between volume and coplanar DBDs. Furthermore, the results showed that plasma mineralization using coplanar DBD can effectively change the energy levels of the surface. This resulted in the enhancement of the work function and the photoelectrochemical properties of the mesoporous TiO₂ photoanodes. This contribution shows that coplanar arrangement of electrodes in DBDs generates plasma of higher efficacy compared with standard volume DBD that is currently often used in industrial processes.     

大气压氖气介质阻挡放电脉冲等离子射流特性

采用自行研制的低造价、小体积、可产生幅值0~35 kV、重复频率1 kHz的高压s脉冲电源,设计了一套以大气压氖气为工作气体的介质阻挡放电（DBD）等离子体射流源,通过测量并计算放电过程中的电压-电流波形、拍摄放电图像、光谱分析等手段,对电压幅值、气体流速对氖气等离子体射流特性的影响进行了研究。结果表明:s脉冲电源激励下大气压氖气DBD能产生锥状的等离子射流且其等离子强度适中;s脉冲电源电压幅值的快速上升,可在放电空间瞬间施加高的过电压,能有效促进放电功率、电子密度、电子激发温度和射流长度的增加;工作气体流速的增加使得放电功率、电子激发温度和电子密度减小,而射流长度变化很小;一定条件下,能形成长距离的射流。     

Langmuir probe and optical emission spectroscopy studies for RF magnetron sputtering during TiON thin film deposition

Low-pressure plasma of gas mixture of Ar, O₂ and N₂ generated by RF magnetron sputtering was characterized by Langmuir probe and optical emission spectroscopy (OES). The electron temperature (T_e), ion density (n_i) and electron energy distribution function (EEDF) in Ar-O₂-N₂ plasma atmosphere were calculated from I-V characteristic of Langmuir probe. Boltzmann plot method was applied for calculating the vibrational temperature (T_vib) of the second positive system of N₂ (N₂SPS) in Ar-O₂-N₂ plasma. The T_e, n_i, EEDF and T_vib in Ar-O₂-N₂ plasma were studied as a function of O₂ percentages. It was found, the T_vib increased from 0.47 eV to 0.55 eV as the oxygen percentage in Ar-N₂-O₂ plasma increased from 10% to 40%. Further, the T_e increased from 1.6 eV to 3 eV as the O₂ concentration increased from 10% to 40%.     

大气压冷等离子体射流研究进展

有许多种方法可用于在大气中产生等离子体射流,冷等离子体（离子温度在室温附近）射流即是其中的一种.近年来,人们发现氦气或其它惰性气体通过毛细管介质阻挡放电形成的冷等离子体射流具有类似子弹的传输特性,在有机材料表面改性、等离子体医学等领域获得了广泛的应用.通过专门设计的一系列实验,我们逐渐揭示了其产生机理,并深入研究了传输特性.文章简要介绍近年来我们所做的有关大气压冷等离子体的实验过程以及获得的一些重要结论.在对这种等离子体深入了解的基础上,作者还开发了一种新装置,该装置的最大特点是既利用了氦气在辅助放电方面的特性,又不消耗这种昂贵的资源;并且它还特别适合于在臭氧层修复、等离子体医学等方面的应用.     

Measurement of C2 and CH temperatures in argon‐acetylene low‐pressure microwave‐induced plasma

The emission spectra of C₂(d³Π_g–a³Π_u), CH(A²Δ–X²Π), and CH(B²Σ–X²Π) bands are analysed to measure rotational T_rot, vibrational T_vib, and gas temperature T_g from Ar/C₂H₂ (5–20% C₂H₂) microwave‐induced plasma (MIP). In case when helium and hydrogen are used in the gas mixture instead of argon, no significant change in T_rot is noticed. Both studied temperatures are insensitive in terms of the C₂H₂ percentage. From CH(0–0, A²Δ–X²Π) band R₂ branch lines, two T_rot (T_rot ～ 520–580 K for J′ = 3–9 and T_rot ～ 1,700–1,800 K for J′ = 10–17) are determined. The lower T_rot equals the T_g (500–700 K) measured from C₂ bands in this study. The H₂ Fulcher‐α diagonal bands are recorded as well in the H₂/C₂H₂ mixtures and T_rot～750–900 K of the H₂ ground state measured. T_vib ～ 6,000 K in Ar/C₂H₂ MIP is calculated from the integral intensity ratio of C₂(2,1) and C₂(3,2) bands.     

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设计建立了同轴圆柱介质阻挡放电线状射流装置,并利用其实现了宽度为50mm的大尺度线状射流,并对射流长度随放电参数的变化进行了研究.研究发现,随气压、流量的增加,射流长度呈先增加后达到饱和;随激励电压的增加,射流长度增加.对氮气射流等离子体进行发射光谱诊断,表明氮气等离子体中主要是氮分子和少量氮原子,并利用光谱拟合得出射流的温度范围为290～350K.     

Investigations on the effect of process parameters on the growth of vertically oriented graphene sheet in plasma-enhanced chemical vapour deposition system

A multistage numerical model comprising the plasma kinetics and surface deposition sub-models is developed to study the influence of process parameters, namely, total gas pressure and input plasma power on the plasma chemistry and growth characteristics of vertically oriented graphene sheets (VOGS) grown in the plasma-enhanced chemical vapour deposition system containing the Ar + H₂ + C₂H₂ reactive gas mixture. The spectral and spatial distributions of temperature and number densities, respectively, of plasma species, that is, charged and neutral species in the plasma reactor, are examined using inductively coupled plasma module of COMSOL Multiphysics 5.2 modelling suite. The numerical data from the computational plasma model are fed as the input parameters for the surface deposition model, and from the simulation results, it is found that there is a significant drop in the densities of various plasma species as one goes from the bulk plasma region to the substrate surface. The significant loss of the energetic electrons is observed in the plasma region at high pressure (for constant input power) and low input power (for constant gas pressure). At low pressure, the carbon species generate at higher rates on the catalyst nanoislands surface, thus enhancing the growth and surface density of VOGS. However, it is found that VOGS growth rate increases when input plasma power is raised from 100 to 300 W and decreases with further increase in the plasma power. A good comparison of the model outcomes with the available experimental results confirms the adequacy of the present model.     

常压射流等离子体发射光谱研究

使用改进介质阻挡放电装置生成常压射流等离子体,采用光纤光栅光谱仪在300～1 000 nm范围记录了不同放电电压的氩气发射光谱,并比较了空气和氩气常压介质阻挡放电等离子体发射光谱,分析发现氩气发射光谱中的谱线都是氩原子的发射谱线,表明常压射流装置产生的等离子体全部为氩等离子体,而无其他空气成分参与放电。为测量电子激发温度,选用相距较近的763.51和772.42 nm两条光谱线对电子温度进行分析,结果表明电子激发温度的范围在0.1～0.3 eV,而且它还随着放电电压的增加而增加。初步使用“红外测温仪”测量被处理材料表面温度,结果发现材料表面的温度也随着放电电压的增加而增加,范围在50～100 ℃,材料表面温度的变化趋势可以近似表征等离子体宏观温度变化趋势。通过分析常压射流等离子体的温度特性,探讨了常压射流等离子体温度对材料改性研究的意义。     

Development of a new atmospheric pressure cold plasma jet generator and application in sterilization

This paper reports that a new plasma generator at atmospheric pressure, which is composed of two homocentric cylindrical all-metal tubes, successfully generates a cold plasma jet. The inside tube electrode is connected to ground, the outside tube electrode is connected to a high-voltage power supply, and a dielectric layer is covered on the outside tube electrode. When the reactor is operated by low-frequency (6 kHz--20 kHz) AC supply in atmospheric pressure and argon is steadily fed as a discharge gas through inside tube electrode, a cold plasma jet is blown out into air and the plasma gas temperature is only 25--30℃. The electric character of the discharge is studied by using digital real-time oscilloscope (TDS 200-Series), and the discharge is capacitive. Preliminary results are presented on the decontamination of E.colis bacteria and Bacillus subtilis bacteria by this plasma jet, and an optical emission analysis of the plasma jet is presented in this paper. The ozone concentration generated by the plasma jet is 1.0×10¹⁶cm^-3 which is acquired by using the ultraviolet absorption spectroscopy.     

大气压下氩原子谱线辐射诊断试验研究

大气压下介质阻挡放电应用领域具有多范畴、深广度、常态化等优势,针对同轴电极放电试验进行了系列参数诊断。采用自主研发的介质阻挡放电助燃激励器,在一个标准大气压、放电频率11.4 kHz、放电峰值电压5.4～13.4 kV(间隔1.0 kV)条件下进行了氩气电离试验。采用原子发射光谱法(AES)对氩等离子体谱线的激发、分光进行了检测分析;选用二谱线法及Boltzmann法测试了电子激励温度;根据Stark展宽效应计算了电子密度;获得了电子激励温度及电子密度随放电峰值电压增长的变化规律。结果表明,在试验电压条件下电子激励温度并不随外加电压的升高而递增,这表明通道内微放电的主要特征并不依赖于外部电压的供给,而是取决于气体组份、气体压强和放电模型,增大外加放电电压仅增加单位时间内微放电的数量,经整合电子激励温度可达3 500 K符合典型的低温等离子体特征;电子密度随外加电压的增长而趋于准线性趋势,电子密度数量级可达到108～109 cm-3,电离度偏弱。这些参数的探索对等离子体研讨有重大意义。     

层流等离子体射流温度与速度测量

本文分别应用光谱诊断、水冷皮托管及小尺寸杆状热流探针,对自由射入空气中的纯氩层流等离子体射流中心最高温度、滞止压力以及最大热流密度进行了测量,由测量结果导出了层流射流的中心最大速度,得到了射流气体温度和速度的轴向分布及其随工作电流和气流量变化的一些规律,探讨了气体的温度和速度对其向探针表面换热系数的影响。     

Determination of the Energy Flux of a Commercial Atmospheric‐Pressure Plasma Jet for Different Process Gases and Distances Between Nozzle Outlet and Substrate Surface

The energy flux of an atmospheric‐pressure plasma jet for surface treatment has been investigated by a calorimetric probe. Generally, the investigations exhibit that the main contributions of the total energy influx from the plasma to the substrate surface originate from the neutrals regarding high gas temperature coupled with a high gas flow. The use of nitrogen as process gas shows a higher energy flux compared to oxygen and air presumably caused by increased gas temperature as well as by higher molecule formation and recombination energy of N₂. Moreover, the lateral expansion of the plasma beam could be roughly determined by a spatially resolved analysis of the energy influx. A top part mounted on the nozzle, commonly used for the injection of additional precursor gases, showed a significant effect on the flow behavior and collision entailed relaxation of the excited plasma species leading to a restraining of the plasma jet. (© 2014 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)     

Surface modification of polypropylene with an atmospheric pressure plasma jet sustained in argon and an argon/water vapour mixture

In this paper, an atmospheric pressure plasma jet sustained in pure argon and an argon/water vapour mixture has been used to modify the surface of polypropylene (PP) films. The gas temperature of the plasma jet was found to be 625 K in an active zone between the electrodes and was found to increase in the afterglow. Based on these results, the PP films are placed as close as possible to the edge of the capillary in order to avoid thermal damage to the polymer. XPS results on the untreated and modified PP samples revealed incorporation of a significant amount of oxygen on the polymer surface, however, this oxygen inclusion is more pronounced for the argon/water vapour jet due to the higher radicals density in the jet afterglow. One can therefore conclude that adding water vapour to an argon plasma jet can be a convenient way to increase the efficiency of plasma surface modification.     

Characteristics of an atmospheric‐pressure radio frequency‐driven Ar/H2 plasma discharge with copper wire in tube

This paper investigates a plasma discharge driven by a 13.56 MHz radio frequency (RF) power supply at atmospheric pressure, in which a copper wire is inserted in the discharge tube for the deposition of Cu films. The results show that the jet plasma formation originates from the discharge between the copper wire and induction coil because of its electrostatic field. The axial distribution of the plasma parameters in the RF plasma jet, namely the gas temperature, excitation temperature, and electron number density, is determined by diatomic molecule OH fitting, Boltzmann slope, and H_β Stark broadening, respectively. The discharge current significantly declines when a small amount of hydrogen is added to the argon as the plasma‐forming gas, and the gas temperature of discharge plasma increases considerably.     

Characterization of an atmospheric pressure plasma jet for surface modification and thin film deposition

In this paper, an experimental study is presented to characterize a commercially available atmospheric pressure plasma jet (APPJ) kINPen which can be used for local surface modification, e.g. changing the wettability as well as for thin film deposition with silicon-organic and metal-organic precursors to enhance scratch resistance or to lower the gas permeability. Characterization of the jet discharge has been carried out by three methods: (i) measurement of the energy influx from the jet plasma to a substrate by a calorimetric probe, (ii) spatial resolved investigation of the plasma beam by optical emission spectroscopy (OES) and (iii) observation of the plasma jet by video imaging. The deposited SiO _x and AlO _x films were analyzed by XPS measurements.     

同轴介质阻挡放电发生器介质层等效电容和负载特性研究

大气压介质阻挡放电(DBD)可以在常压下产生非平衡等离子体,已经成为热点研究领域.通过脉冲或交变电源激发放电,研究电源输出特性、电源与放电发生器负载间的匹配和外界条件对放电的影响对于理解放电现象和提高放电效率具有重要意义.本文采用Lissajous图形法,分别研究了驱动电压、气流速率等因素影响同轴DBD发生器介质层等效电容及负载幅频特性的规律.结果表明,气流速率和驱动电压等外界条件影响DBD发生器的负载特性:介质层等效电容随气流速率增大而减小,随驱动电压增大而增大;幅频特性曲线均表现出RLC回路谐振现象,谐振频率随气流速率增大而增大,随驱动电压增大而减小.通过对比发现,介质层等效电容随频率的变化曲线与幅频特性曲线具有一致的特征,介质层等效电容是影响电路谐振频率动态变化的主要因素.提出了一种有关介质层等效电容的形成机制.     

Effect of reactor surface modification on the neutral gas temperature in a transformer-coupled toroidal plasma

Transformer-coupled toroidal plasma (TCTP) has found applications in versatile fields as a high-power-density plasma source. However, most research on TCTP has focused on plasma states in the TCTP, without any change in reactor structures. Therefore, in this paper, we present a study on the effects of inner-surface modification of a TCTP reactor on plasma conditions. Using two types of reactors with different inner surfaces, the silicon-wafer etch rate by fluorine atoms from dissociated NF₃ gas molecules is compared. Then a computer simulation, which derives various plasma parameters, is carried out. As a result, the TCTP reactor with a grooved inner surface shows a higher etch rate than the reactor with a normal inner surface. The computer simulation suggests the reason for this etch rate difference is that the reactor with the grooved inner surface structure has a higher neutral gas temperature than the reactor with the normal inner surface so that more pyrolytic dissociation, resulting in a higher fluorine atom density, is achieved. Our results may be useful for those fields that require a higher neutral temperature or a higher degree of pyrolysis.