滑动弧放电等离子体降解气相及液相中有机污染物的研究
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摘要
滑动弧放电是一种大气压下非热等离子体，该技术产生的基本原理是在一对电极间加上电压并通过气流，在电极之间最窄处形成放电弧，利用气流来推动电弧，使它向下游移动同时电弧的长度随着电极间距离的增大而增加，当电弧长度达到临界值时消失，同时在电极最窄处形成新的电弧，重复上述过程形成放电。滑动弧放电的主要特点是：兼具热等离子体和非热等离子体的特性；滑动弧放电装置和电源结构简单、价格低廉、操作和维护费用比较；电极不需要冷却，并且能够自清洁，不易腐蚀和消蚀，使用寿命长；电能直接进入反应区域，产生一个充满活性粒子的非平衡态等离子体反应环境，超过80％的电能直接被化学反应吸收；进气不需要预处理，可以用多相体(气液混合相、气固混合相、气液固混合相)反应。本文主要开展了滑动弧放电等离子体降解气相及液相中有机污染物的研究。
首先，设计了气相滑动弧放电发生器和气液两相滑动弧放电发生器，对它们进行了电信号测量、图像测量和温度测量。根据电参数、图像分析结果及Elenbass-Heller方程建立了滑动电弧等离子体通道Elenbass-Heller模型，并计算了电场强度和电子密度等参数。根据滑动放电等离子体的化学特性，研究并总结了湿空气低温等离子体和气液两相滑动弧放电等离子体化学反应动力学模型。分析了自由基氧化有机物的机理，并通过烷烃、醛和酸等实例加以说明。
利用实验室规模的气相滑动弧放电反应器探讨了操作参数变化对低温等离子体系统的影响。在去除甲苯的实验中发现：许多操作参数会影响低温等离子体对挥发性有机物的去除率，其中，去除率随施加电压、输入体积能耗、氧气含量、水汽浓度、气流温度及停留时间的增加而增大，随初始浓度的增加而减小。当电压升到10kV时，甲苯的去除率达到90％；分析了~·OH、O_2、NO和O_3等活性粒子氧化甲苯的路径。在脱除烟气中多环芳烃和碳黑颗粒的过程中发现：滑动弧放电可有效同时脱除PE和PVC焚烧烟气中的PAHs和碳黑颗粒；烟气经过滑动弧放电处理后，PAHs达到最高脱除率74.4％，碳黑达到最高脱除率为89.3％；分析了PAHs和碳黑颗粒的降解路径。并根据滑动弧放电等离子体适于降解高浓度有机物废气的特性，结合活性炭吸附法，提出了吸附器的吸附浓缩和热脱附一等离子体净化技术。
利用气液两相滑动弧放电Ⅰ型反应器开展了降解200mg／1苯酚模拟废水的初
The gliding arc (glidarc) discharge is considered to be a non-thermal plasma. Gliding discharge is produced between at least two diverging electrodes and across the flow, self-initiated in the upstream narrowest gap, the discharge forms the plasma column connecting the electrodes. This column is dragged by the flow towards the diverging downstream section. The discharge length grows with the increase of inter-electrode distance until it reaches a critical value. After this point, the discharge extinguishes but momentarily reignites itself at the minimum distance between the electrodes and a new cycle starts. The main advantages of gliding arc discharge are: having a dual character of thermal and non-thermal plasma; inexpensive both from capital and operating costs; The electrodes do not need to be cooled, the discharges perform their own maintenance on the electrodes, preventing chemical corrosion and erosion; the electrical energy is directly introduced into the reaction volume to create a non-equilibrium and very reactive environment for promoting the chemical transformations of interest; any gas, gas-liquid, gas-solid or gas-liquid-solid can be directly processed; any initial gas temperature can be accepted. This paper presents experimental results on the degradation of organic contaminations from gas and liquid phase using gliding arc discharge plasma
Firstly, two plasma generators (gas and gas-liquid gliding arc) are designed in our laboratory with the aim to obtain the physical and chemical characteristics, several diagnostic methods are used (high speed photography with a CCD camera, electric measurements, temperature measurements). Based on physical experimental results and Elenbass-Heller equation, a simple theoretical plasma channel model of gliding arc is given which enables determination of the electronic density and electric field strength. Based on the chemical characteristics of gliding arc discharge and the model of Peyrou R., the chemical kinetics of humid air and gas-liquid gliding arc discharges is modeled. The degradation mechanisms of hydrocarbons with polyfunctional groups like carboxyl-, aldehyde-, ketone- or alkanol- groups are introduced.
Laboratory-scale gas glidarc reactors are constructed and used to investigate the effects of operational parameters on volatile organic compounds (VOCs) removal efficiencies. Experimental results of toluene removal indicate that many factors will
首先，设计了气相滑动弧放电发生器和气液两相滑动弧放电发生器，对它们进行了电信号测量、图像测量和温度测量。根据电参数、图像分析结果及Elenbass-Heller方程建立了滑动电弧等离子体通道Elenbass-Heller模型，并计算了电场强度和电子密度等参数。根据滑动放电等离子体的化学特性，研究并总结了湿空气低温等离子体和气液两相滑动弧放电等离子体化学反应动力学模型。分析了自由基氧化有机物的机理，并通过烷烃、醛和酸等实例加以说明。
利用实验室规模的气相滑动弧放电反应器探讨了操作参数变化对低温等离子体系统的影响。在去除甲苯的实验中发现：许多操作参数会影响低温等离子体对挥发性有机物的去除率，其中，去除率随施加电压、输入体积能耗、氧气含量、水汽浓度、气流温度及停留时间的增加而增大，随初始浓度的增加而减小。当电压升到10kV时，甲苯的去除率达到90％；分析了~·OH、O_2、NO和O_3等活性粒子氧化甲苯的路径。在脱除烟气中多环芳烃和碳黑颗粒的过程中发现：滑动弧放电可有效同时脱除PE和PVC焚烧烟气中的PAHs和碳黑颗粒；烟气经过滑动弧放电处理后，PAHs达到最高脱除率74.4％，碳黑达到最高脱除率为89.3％；分析了PAHs和碳黑颗粒的降解路径。并根据滑动弧放电等离子体适于降解高浓度有机物废气的特性，结合活性炭吸附法，提出了吸附器的吸附浓缩和热脱附一等离子体净化技术。
利用气液两相滑动弧放电Ⅰ型反应器开展了降解200mg／1苯酚模拟废水的初
The gliding arc (glidarc) discharge is considered to be a non-thermal plasma. Gliding discharge is produced between at least two diverging electrodes and across the flow, self-initiated in the upstream narrowest gap, the discharge forms the plasma column connecting the electrodes. This column is dragged by the flow towards the diverging downstream section. The discharge length grows with the increase of inter-electrode distance until it reaches a critical value. After this point, the discharge extinguishes but momentarily reignites itself at the minimum distance between the electrodes and a new cycle starts. The main advantages of gliding arc discharge are: having a dual character of thermal and non-thermal plasma; inexpensive both from capital and operating costs; The electrodes do not need to be cooled, the discharges perform their own maintenance on the electrodes, preventing chemical corrosion and erosion; the electrical energy is directly introduced into the reaction volume to create a non-equilibrium and very reactive environment for promoting the chemical transformations of interest; any gas, gas-liquid, gas-solid or gas-liquid-solid can be directly processed; any initial gas temperature can be accepted. This paper presents experimental results on the degradation of organic contaminations from gas and liquid phase using gliding arc discharge plasma
Firstly, two plasma generators (gas and gas-liquid gliding arc) are designed in our laboratory with the aim to obtain the physical and chemical characteristics, several diagnostic methods are used (high speed photography with a CCD camera, electric measurements, temperature measurements). Based on physical experimental results and Elenbass-Heller equation, a simple theoretical plasma channel model of gliding arc is given which enables determination of the electronic density and electric field strength. Based on the chemical characteristics of gliding arc discharge and the model of Peyrou R., the chemical kinetics of humid air and gas-liquid gliding arc discharges is modeled. The degradation mechanisms of hydrocarbons with polyfunctional groups like carboxyl-, aldehyde-, ketone- or alkanol- groups are introduced.
Laboratory-scale gas glidarc reactors are constructed and used to investigate the effects of operational parameters on volatile organic compounds (VOCs) removal efficiencies. Experimental results of toluene removal indicate that many factors will
引文
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