大气压纳秒脉冲介质阻挡放电光谱特性与应用基础研究
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摘要
纳秒脉冲介质阻挡放电因具有能量利用率高、均匀性好、等离子体电子温度高和气体温度接近室温等优点,成为近年来的研究热点。本文在大气压氮气和空气中利用具有20ns上升沿的双极性纳秒脉冲电源,在针-板、多针-板和板-板电极结构中产生了弥散介质阻挡放电等离子体,主要研究内容如下：
1.针-板电极结构中,在大气压空气中利用双极性纳秒脉冲介质阻挡放电产生了气体温度接近室温的弥散等离子体。在强电磁干扰环境下测量了纳秒脉冲放电等离子体的发射光谱、N2(C3Πu→B3Πg,0-0)光电流波形和脉冲电压波形,利用N2+(B2Σu+→X2Σg+0-0)发射光谱拟合计算了纳秒脉冲放电等离子体气体温度,通过N2(C→B)光电流波形与脉冲电压波形讨论了双极性纳秒脉冲介质阻挡放电机理,并研究了脉冲峰值电压、脉冲重复频率、电极间隙和空气中O2对放电均匀性、等离子体气体温度和发射光谱特性的影响。结果表明,双极性纳秒脉冲放电中正脉冲放电只出现一次主要放电,N2(C→B)光电流波形中出现一个滞后电压脉冲峰约80ns、脉宽约50-60ns的光电流强度峰,N2(C→B)光电流峰与脉冲电压峰的滞后时间随电压增长保持不变；负脉冲放电中,N2(C→B)光电流峰出现在脉冲下降沿的拖尾上,当脉冲峰值电压为16kV时,N2(C→B)光电流峰与脉冲电压峰的滞后时间是正脉冲放电中的50倍,且滞后时间随着脉冲峰值电压的升高而迅速缩短。
2.通过增加针电极数量,在大气压空气中实现了较大面积的弥散双极性纳秒脉冲介质阻挡放电等离子体,并研究了针-板电极间隙、脉冲峰值电压和脉冲重复频率对等离子体分布面积、等离子体气体温度等特性和N2(C→B)发射光谱强度在水平方向上空间分布的影响。研究表明双针-板电极结构纳秒脉冲介质阻挡放电的放电体积随脉冲峰值电压的升高而增大,但随脉冲重复频率的升高基本保持不变。值得一提的是,双针-板和多针-板板电极结构下弥散型放电可以在每个针与板之间间距不相等的情况下产生,放电在各个针-板间隙相对独立,可应用于不平整材料表面改性。
3.板-板电极结构中,利用双极性纳秒脉冲电压来驱动产生大气压氮气和空气中稳定的双极性纳秒脉冲均匀介质阻挡放电等离子体。在强电磁干扰的情况下,测量了纳秒脉冲均匀放电图像及单脉冲放电图像、脉冲电压波形、电流波形、光电流波形和等离子体发射光谱,通过N2(C→B)发射光谱拟合计算了等离子体的气体温度,利用脉冲电压波形、电流波形和光电流波形分析了双极性纳秒脉冲介质阻挡放电的击穿机理,研究了脉冲峰值电压、脉冲重复频率和电极间隙对等离子体气体温度和NO (A2Σ→X2Π)、OH(A2Σ→X2Π)、N2(C3Π→B3Πg)发射光谱强度和的影响。结果表明,纳秒脉冲放电脉冲峰值电压、脉冲重复频率和电极间隙对等离子体气体温度存在较小的影响,气体温度随脉冲峰值电压、脉冲重复频率和电极间隙的升高或增加出现轻微升高,但始终保持在接近室温的范围内。NO(A→X)、OH(A→X)和N2(C→B)发射光谱强度均随脉冲峰值电压和脉冲重复频率的升高而增强；当电极间隙为2.5mm时,NO(A→X)、OH(A→X)和N(C→B)发射光谱强度出现极大值,当电极间隙大于2.5mm时,NO(A→X)、OH(A→X)和N2(C→B)发射光谱强度随电极间隙的增大而减小。论文还讨论了O2对大气压氮气均匀纳秒脉冲放电的影响,O2对介质阻挡放电的均匀性和放电强度存在明显的抑制作用,但是,少量O2(03%)的加入可以促进等离子体中NO、OH等活性成分的产生。
4.利用板-板电极结构和针-管电极结构,成功的在大气压空气中产生了均匀的双极性纳秒脉冲介质阻挡放电,并分别应用于提高丙纶(PP)无纺布表面亲水性和真菌、放线菌的杀灭处理上。板-板电极结构中,大气压空气中均匀纳秒脉冲介质阻挡放电可以在3mm的电极间隙下产生,与传统的正弦交流介质阻挡放电相比,纳秒脉冲介质阻挡放电具有较好的均匀性和较高的能量利用率,处理丙纶无纺布使表面水接触角由150°降至110°,纳秒脉冲介质阻挡放电平均注入能量密度不足正弦交流介质阻挡放电的1/20,且对材料表面无任何损伤。通过利用特殊的电极结构,在石英瓶和培养皿内部产生了弥散的双极性纳秒脉冲放电,并实现对培养液和固体附着物的高效杀菌,该结构实验装置成功的应用于华北制药集团培养液和纱布中的真菌、放线菌灭杀上,具备杀菌效率高、需要时间短等优点。
5.利用在大气压He中获得的较大电极间隙中的均匀介质阻挡放电等离子体,测量了大气压He均匀介质阻挡放电发射光谱及He(3s3S→2p3P)、N2(C→B)、N2÷(B→X)和OH(A→X)空间分辨光谱及归一化空间分布,研究了应用电压和驱动频率对He(3s3S→2p3P)发射光谱强度空间分布特性的影响,利用归一化空间分辨光谱讨论了OH、N2+等激发态离子的主要生成和淬灭机制,并从实验上验证了大气压He均匀介质阻挡放电中不对称模式的存在。结果表明He(3s3S→2p3P)、N2(C→B)、 N2+(B→X)和OH(A→X)光谱发射强度在距离上电极1mm和6mm处出现两个最大值,这两个位置的发射光谱强度是距离上电极3-4mm处发射光谱强度的2-3倍。杂质气体(N2)的加入可以导致大气压He均匀介质阻挡放电的模式发生变化,当N2浓度为百ppm量级时,尽管采用了对称的电极结构,正半周期的放电电流幅值要明显大于负半轴的幅值,与之对应的,He(3s3S→2p3P)、N2(C→B)、N2+(B→X)和OH(A→X)发射光谱强度空间分布也出现不对称结构。
Nanosecond pulsed discharge plasma has become a hot field in low temperature non-thermal equilibrium plasma area because of its unique advantages such as high energy effective, good discharge uniformity, high electron temperature and low gas temperature. In this paper, bipolar nanosecond high voltage pulse with20ns rising time is employed to generated uniform or diffuse dielectric barrier discharge using needle-plate, multiple needle-plate, and plate-plate electrode configurations in nitrogen and air at atmospheric pressure. The main research content is described as follow:
1. In needle-needle electrode configuration, bipolar nanosecond pulse voltage is employed to generate diffuse dielectric barrier discharge plasma with low gas temperature. The diffuse dielectric barrier discharge can be obtained in large range of electrode gap distance, pulse peak voltage, and pulse repetition rate. The optical emission spectra, the time resolved spectra of N2(C3Πu→B3Πg,0-0,337.1nm) and the waveform of are recorded under severe electromagnetic interference. The gas temperature is calculated by fitting the first negative bands of N2+(B2Σu→X2Σg+,0-0). It is found that there are two different breakdown modes existing in positive and negative pulse discharges. In positive pulse discharge, the lagged time between the photocurrent pulse and the voltage pulse is about80ns and keep almost constant with the rising of pulse peak voltage. However, in negative pulse discharge the lagged time is much longer and decreases sharply with the rising of pulse peak voltage. In addition, the effect of oxygen in air on the diffuse discharge is studied; it is found the oxygen is not benefit to improve both the uniformity and the discharge intensity in nanosecond pulsed dielectric barrier discharge.
2. Large area air diffuse nanosecond pulsed discharge can be obtained by using double needle-plate and multiple needle-plate electrode configurations at atmospheric pressure. Both double needles and multiple needles electrode configurations nanosecond pulsed dielectric barrier discharge are investigated. It is found that plasma volume increase with the rising of the pulse peak voltage but keep almost content as increasing of pulse repetition rate. In addition, both double needle-plate and multiple needle-plate electrode configurations with different needle-plate electrode gaps are also employed to generate diffuse discharge plasma. It is found that the equivalent needle-plate electrode gap is unnecessary in nanosecond pulsed dielectric barrier discharge, which show the discharge can be used in the material modification of topographically non-uniform surface.
3. In plate-plate electrode configuration, a homogenous dielectric barrier discharge plasma with very low gas temperature is obtained by using nanosecond bipolar pulse voltage with20ns rising time both in nitrogen and air at atmospheric pressure. The images of the discharge, the waveforms of pulse voltage and discharge current, and the optical emission spectra emitted from the discharge are recorded successfully under severe electromagnetic interference. The effects of the pulse peak voltage, the pulse repetition rate, and the gap distance between electrodes on the gas temperature and the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) are discussed. It is found that the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) rise with increasing both the pulse peak voltage and the pulse repetition rate but decrease with gap distance between the electrodes when it is larger than2.5mm. The effect of concentrations of O2on the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) are also investigated, and it is found both the emission intensities of NO (A2Σ→X2Π) and OH (A2Σ→X2Π) reach maximum values when O2concentration is0.3.
4. Nanosecond pulsed discharge is used for surface modification of polypropylene non-woven fabric and plasma mutagenesis of fungi and actinomycetes at atmospheric pressure. In the treatment of polypropylene non-woven fabric, compared with the DBD plasma excited by sine AC voltage, the nanosecond pulsed dielectric barrier discharge exhibits obvious advantages in improving the hydrophilic property of polypropylene non-woven fabric. The average energy cost is about20times lower than AC dielectric barrier discharge for improving the hydrophilic property of polypropylene to the same level. In particular, nanosecond pulsed dielectric barrier discharge plasma can treat the polypropylene non-woven fabric without any surface damage. In the plasma mutagenesis of microorganism, needle-cuvette and plate-plate electrode nanosecond pulsed dielectric barrier discharge plasma source are designed, and they are used to mutagenesis of fungi and actinomycetes in liquid state and solid state respectively for North China Pharmaceutical Co. Ltd..
5. Homogenous dielectric barrier discharge is obtained in Helium at atmospheric pressure and the spatially resolved spectra of He (3s3S→2p3P), OH (A2Σ→X2Π), N2(C3Πu-> B3Πg), and N2+(B2Σu→X2Σ+) emitted from homogeneous dielectric barrier discharge are recorded. The effects of applied voltage and driving frequency on the spatially resolved spectra of I Ie (3s3S→2p3P) are investigated, the formation mechanism of OH and N2+by the impurity in helium are discussed. It is found that the spatial distributions of the emission intensities of He(3s3S→2p3P), OH(A2Σ→X2Π), N2(C3Πu→B3Πg), and N2+(B2Σu+→X2Σg+) exhibit two peaks at1and6mm from the upper electrode respectively in the7mm gas gap and the emission intensities at1and6mm are about2-3times higher than those at3-4mm, and most of the active particles are produced in the two regions. In addition, the impurity adding can lead to the change of discharge mode, when the concentration is in several hundred ppm, when the concentration is in several hundred ppm, the amplitude of the current pulse at the positive half-cycle is larger than that at the negative half-cycle, corresponsively, the asymmetric mode is presented by the spatial distributions of emission intensities of He(3s3S→2p3P), OH(A2E→X2Π), N2(C3Πu→B3Πg), and N2+(B2Σu+→X2Σg+).
1.针-板电极结构中,在大气压空气中利用双极性纳秒脉冲介质阻挡放电产生了气体温度接近室温的弥散等离子体。在强电磁干扰环境下测量了纳秒脉冲放电等离子体的发射光谱、N2(C3Πu→B3Πg,0-0)光电流波形和脉冲电压波形,利用N2+(B2Σu+→X2Σg+0-0)发射光谱拟合计算了纳秒脉冲放电等离子体气体温度,通过N2(C→B)光电流波形与脉冲电压波形讨论了双极性纳秒脉冲介质阻挡放电机理,并研究了脉冲峰值电压、脉冲重复频率、电极间隙和空气中O2对放电均匀性、等离子体气体温度和发射光谱特性的影响。结果表明,双极性纳秒脉冲放电中正脉冲放电只出现一次主要放电,N2(C→B)光电流波形中出现一个滞后电压脉冲峰约80ns、脉宽约50-60ns的光电流强度峰,N2(C→B)光电流峰与脉冲电压峰的滞后时间随电压增长保持不变；负脉冲放电中,N2(C→B)光电流峰出现在脉冲下降沿的拖尾上,当脉冲峰值电压为16kV时,N2(C→B)光电流峰与脉冲电压峰的滞后时间是正脉冲放电中的50倍,且滞后时间随着脉冲峰值电压的升高而迅速缩短。
2.通过增加针电极数量,在大气压空气中实现了较大面积的弥散双极性纳秒脉冲介质阻挡放电等离子体,并研究了针-板电极间隙、脉冲峰值电压和脉冲重复频率对等离子体分布面积、等离子体气体温度等特性和N2(C→B)发射光谱强度在水平方向上空间分布的影响。研究表明双针-板电极结构纳秒脉冲介质阻挡放电的放电体积随脉冲峰值电压的升高而增大,但随脉冲重复频率的升高基本保持不变。值得一提的是,双针-板和多针-板板电极结构下弥散型放电可以在每个针与板之间间距不相等的情况下产生,放电在各个针-板间隙相对独立,可应用于不平整材料表面改性。
3.板-板电极结构中,利用双极性纳秒脉冲电压来驱动产生大气压氮气和空气中稳定的双极性纳秒脉冲均匀介质阻挡放电等离子体。在强电磁干扰的情况下,测量了纳秒脉冲均匀放电图像及单脉冲放电图像、脉冲电压波形、电流波形、光电流波形和等离子体发射光谱,通过N2(C→B)发射光谱拟合计算了等离子体的气体温度,利用脉冲电压波形、电流波形和光电流波形分析了双极性纳秒脉冲介质阻挡放电的击穿机理,研究了脉冲峰值电压、脉冲重复频率和电极间隙对等离子体气体温度和NO (A2Σ→X2Π)、OH(A2Σ→X2Π)、N2(C3Π→B3Πg)发射光谱强度和的影响。结果表明,纳秒脉冲放电脉冲峰值电压、脉冲重复频率和电极间隙对等离子体气体温度存在较小的影响,气体温度随脉冲峰值电压、脉冲重复频率和电极间隙的升高或增加出现轻微升高,但始终保持在接近室温的范围内。NO(A→X)、OH(A→X)和N2(C→B)发射光谱强度均随脉冲峰值电压和脉冲重复频率的升高而增强；当电极间隙为2.5mm时,NO(A→X)、OH(A→X)和N(C→B)发射光谱强度出现极大值,当电极间隙大于2.5mm时,NO(A→X)、OH(A→X)和N2(C→B)发射光谱强度随电极间隙的增大而减小。论文还讨论了O2对大气压氮气均匀纳秒脉冲放电的影响,O2对介质阻挡放电的均匀性和放电强度存在明显的抑制作用,但是,少量O2(03%)的加入可以促进等离子体中NO、OH等活性成分的产生。
4.利用板-板电极结构和针-管电极结构,成功的在大气压空气中产生了均匀的双极性纳秒脉冲介质阻挡放电,并分别应用于提高丙纶(PP)无纺布表面亲水性和真菌、放线菌的杀灭处理上。板-板电极结构中,大气压空气中均匀纳秒脉冲介质阻挡放电可以在3mm的电极间隙下产生,与传统的正弦交流介质阻挡放电相比,纳秒脉冲介质阻挡放电具有较好的均匀性和较高的能量利用率,处理丙纶无纺布使表面水接触角由150°降至110°,纳秒脉冲介质阻挡放电平均注入能量密度不足正弦交流介质阻挡放电的1/20,且对材料表面无任何损伤。通过利用特殊的电极结构,在石英瓶和培养皿内部产生了弥散的双极性纳秒脉冲放电,并实现对培养液和固体附着物的高效杀菌,该结构实验装置成功的应用于华北制药集团培养液和纱布中的真菌、放线菌灭杀上,具备杀菌效率高、需要时间短等优点。
5.利用在大气压He中获得的较大电极间隙中的均匀介质阻挡放电等离子体,测量了大气压He均匀介质阻挡放电发射光谱及He(3s3S→2p3P)、N2(C→B)、N2÷(B→X)和OH(A→X)空间分辨光谱及归一化空间分布,研究了应用电压和驱动频率对He(3s3S→2p3P)发射光谱强度空间分布特性的影响,利用归一化空间分辨光谱讨论了OH、N2+等激发态离子的主要生成和淬灭机制,并从实验上验证了大气压He均匀介质阻挡放电中不对称模式的存在。结果表明He(3s3S→2p3P)、N2(C→B)、 N2+(B→X)和OH(A→X)光谱发射强度在距离上电极1mm和6mm处出现两个最大值,这两个位置的发射光谱强度是距离上电极3-4mm处发射光谱强度的2-3倍。杂质气体(N2)的加入可以导致大气压He均匀介质阻挡放电的模式发生变化,当N2浓度为百ppm量级时,尽管采用了对称的电极结构,正半周期的放电电流幅值要明显大于负半轴的幅值,与之对应的,He(3s3S→2p3P)、N2(C→B)、N2+(B→X)和OH(A→X)发射光谱强度空间分布也出现不对称结构。
Nanosecond pulsed discharge plasma has become a hot field in low temperature non-thermal equilibrium plasma area because of its unique advantages such as high energy effective, good discharge uniformity, high electron temperature and low gas temperature. In this paper, bipolar nanosecond high voltage pulse with20ns rising time is employed to generated uniform or diffuse dielectric barrier discharge using needle-plate, multiple needle-plate, and plate-plate electrode configurations in nitrogen and air at atmospheric pressure. The main research content is described as follow:
1. In needle-needle electrode configuration, bipolar nanosecond pulse voltage is employed to generate diffuse dielectric barrier discharge plasma with low gas temperature. The diffuse dielectric barrier discharge can be obtained in large range of electrode gap distance, pulse peak voltage, and pulse repetition rate. The optical emission spectra, the time resolved spectra of N2(C3Πu→B3Πg,0-0,337.1nm) and the waveform of are recorded under severe electromagnetic interference. The gas temperature is calculated by fitting the first negative bands of N2+(B2Σu→X2Σg+,0-0). It is found that there are two different breakdown modes existing in positive and negative pulse discharges. In positive pulse discharge, the lagged time between the photocurrent pulse and the voltage pulse is about80ns and keep almost constant with the rising of pulse peak voltage. However, in negative pulse discharge the lagged time is much longer and decreases sharply with the rising of pulse peak voltage. In addition, the effect of oxygen in air on the diffuse discharge is studied; it is found the oxygen is not benefit to improve both the uniformity and the discharge intensity in nanosecond pulsed dielectric barrier discharge.
2. Large area air diffuse nanosecond pulsed discharge can be obtained by using double needle-plate and multiple needle-plate electrode configurations at atmospheric pressure. Both double needles and multiple needles electrode configurations nanosecond pulsed dielectric barrier discharge are investigated. It is found that plasma volume increase with the rising of the pulse peak voltage but keep almost content as increasing of pulse repetition rate. In addition, both double needle-plate and multiple needle-plate electrode configurations with different needle-plate electrode gaps are also employed to generate diffuse discharge plasma. It is found that the equivalent needle-plate electrode gap is unnecessary in nanosecond pulsed dielectric barrier discharge, which show the discharge can be used in the material modification of topographically non-uniform surface.
3. In plate-plate electrode configuration, a homogenous dielectric barrier discharge plasma with very low gas temperature is obtained by using nanosecond bipolar pulse voltage with20ns rising time both in nitrogen and air at atmospheric pressure. The images of the discharge, the waveforms of pulse voltage and discharge current, and the optical emission spectra emitted from the discharge are recorded successfully under severe electromagnetic interference. The effects of the pulse peak voltage, the pulse repetition rate, and the gap distance between electrodes on the gas temperature and the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) are discussed. It is found that the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) rise with increasing both the pulse peak voltage and the pulse repetition rate but decrease with gap distance between the electrodes when it is larger than2.5mm. The effect of concentrations of O2on the emission intensities of NO (A2Σ→X2Π), OH (A2Σ→X2Π), and N2(C3Πu→B3Πg) are also investigated, and it is found both the emission intensities of NO (A2Σ→X2Π) and OH (A2Σ→X2Π) reach maximum values when O2concentration is0.3.
4. Nanosecond pulsed discharge is used for surface modification of polypropylene non-woven fabric and plasma mutagenesis of fungi and actinomycetes at atmospheric pressure. In the treatment of polypropylene non-woven fabric, compared with the DBD plasma excited by sine AC voltage, the nanosecond pulsed dielectric barrier discharge exhibits obvious advantages in improving the hydrophilic property of polypropylene non-woven fabric. The average energy cost is about20times lower than AC dielectric barrier discharge for improving the hydrophilic property of polypropylene to the same level. In particular, nanosecond pulsed dielectric barrier discharge plasma can treat the polypropylene non-woven fabric without any surface damage. In the plasma mutagenesis of microorganism, needle-cuvette and plate-plate electrode nanosecond pulsed dielectric barrier discharge plasma source are designed, and they are used to mutagenesis of fungi and actinomycetes in liquid state and solid state respectively for North China Pharmaceutical Co. Ltd..
5. Homogenous dielectric barrier discharge is obtained in Helium at atmospheric pressure and the spatially resolved spectra of He (3s3S→2p3P), OH (A2Σ→X2Π), N2(C3Πu-> B3Πg), and N2+(B2Σu→X2Σ+) emitted from homogeneous dielectric barrier discharge are recorded. The effects of applied voltage and driving frequency on the spatially resolved spectra of I Ie (3s3S→2p3P) are investigated, the formation mechanism of OH and N2+by the impurity in helium are discussed. It is found that the spatial distributions of the emission intensities of He(3s3S→2p3P), OH(A2Σ→X2Π), N2(C3Πu→B3Πg), and N2+(B2Σu+→X2Σg+) exhibit two peaks at1and6mm from the upper electrode respectively in the7mm gas gap and the emission intensities at1and6mm are about2-3times higher than those at3-4mm, and most of the active particles are produced in the two regions. In addition, the impurity adding can lead to the change of discharge mode, when the concentration is in several hundred ppm, when the concentration is in several hundred ppm, the amplitude of the current pulse at the positive half-cycle is larger than that at the negative half-cycle, corresponsively, the asymmetric mode is presented by the spatial distributions of emission intensities of He(3s3S→2p3P), OH(A2E→X2Π), N2(C3Πu→B3Πg), and N2+(B2Σu+→X2Σg+).
引文
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