滑动弧放电等离子体降解芳香烃类有机污染物的基础研究
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摘要
随着工业生产的发展和生活质量的提高,人类在生产和生活过程中不可避免地排放出各种污染物,对环境造成了各种不同程度的威胁。其中,由于芳烃类有机污染物对环境的污染尤为严重。各国科学家正在研究不同的技术对这类污染物的排放进行控制。相对常规方法,非平衡等离子体技术具有其独特的优点：能提供大量的高能电子,各种活性自由基,紫外线等。因此这种技术受到广泛关注,被视为环境治理的潜在技术之一。本文将一种新型的非平衡等离子体技术——滑动弧等离子体技术用于三类芳烃类污染物的降解。在充分认识滑动弧等离子体的基本物理特性基础上,研究利用其降解多环芳烃、1,2-二氯苯和飞灰中二恶英的过程,认识这些污染物的降解机理。本文的主要研究内容如下：
(一)对研究相关背景和相关知识的文献综述。分别介绍了论文中的处理对象多环芳烃,氯苯和二恶英的基本物理化学性质,对环境的危害以及现有的处理方法。另外,对等离子体的定义和分类,非平衡等离子体的发生方式,以及非平衡等离子体技术在环境治理方面的应用进行了介绍。最后,对本文中所使用的滑动弧等离子技术的研究报道进行了充分综述,包括其物理化学特性,其在环境治理和能源转换,材料处理等方面的应用等。
(二)滑动弧等离子体的物理特性研究。分析滑动弧放电在不同工作条件下的电参数特性。并通过利用快速傅立叶变换方法分析电压信号获取等离子体的脉动的频率特性。利用光栅光谱仪检测了不同实验条件下的滑动弧放等离子体中的发射光谱,检测了在不同的气氛下,滑动弧产生的主要自由基,以及在反应器中自由基的轴向分布。另外,对新近发展龙旋风滑动弧反应器的工作特性进行了研究。分析了在不同实验工况下的电参数特性；研究了在不同流量配置下等离子体物理特性的变化,并基于以上分析总结了龙旋风滑动弧等离子体反应器的三种工作模式,找到了稳定的工作模式。
(三)利用滑动弧等离子体降解多环芳烃的研究。首先以萘为降解对象,研究了等离子体发生电路外部电阻、载气种类和萘的初始浓度对降解过程的影响。结果表明萘的降解率最高可达92.3%。降解率随着氧气浓度的增加而增加,随着外部电阻减小而增加。能量效率最高可达3.6g/kWh。降解能量效率随着外部电阻增大而明显增大。另外,检测了在不同气氛放电中的降解产物,通过分析降解产物分析萘在不同气氛放电中降解的主要机理。为了提高处理多环芳烃过程的能量效率,本文还研究了利用滑动弧同时脱除多种多环芳烃(二氢苊、芴、蒽和芘)过程。
(四)臭氧辅助滑动弧等离子体降解1,2-二氯苯的研究。分析滑动弧等离子体工作条件中的关键参数对1,2-二氯苯降解过程的影响。结果表明,1,2-二氯苯的降解率相对偏低,当外部电阻为50kΩ,载气为氧气时,降解率最高可达74.1%。通过检测在不同气氛下的主要降解产物,研究1,2-二氯苯的降解机理。为了提高1,2-二氯苯的降解率,本文利用臭氧辅助滑动弧对1,2-二氯苯进行降解。研究了臭氧在等离子体区域和后等离子体区域的作用以及气氛对这种新方法的影响。结果表明,只有在氮气和氧气等离子体放电下,在后等离子体区域同入臭氧才能够提高1,2-二氯苯的降解率。
(五)利用龙旋风滑动弧反应器降解垃圾焚烧飞灰中二恶英的研究。当载气为氧气时,飞灰中二恶英的降解率达到最高,二恶英的质量降解率为67.7%,毒性当量降解率为72.3%,降解后飞灰中的二恶英浓度为638pg-TEQ/g,尾气中二恶英的浓度为342pg-TEQ/Nm3。通过分析处理前后飞灰和尾气中二恶英同系物的分布以及飞灰表面形态变化,初步提出飞灰中二恶英的降解途径：一是等离子体直接作用于飞灰表面,实现二恶英的降解。二是飞灰中二恶英挥发之气相中,通过与等离子体中的高活性基团发生气相反应,实现降解的过程。
With the development of industry and improvement of life quality, release of kinds of pollutants to the environment is inevitable, which results in threats to the whole environment. Among of them, pollutions by Aromatic Hydrocarbon Organic Pollutants (AHOPs) are very serous. Scientists dedicate to invent and develop different technologies to control AHOPs emission. Compared with traditional methods, nonthermal plasma has some unique advantages that providing numerous free radicals and energetic electrons, low gas temperature and so on. Therefore, nonthermal plasma is received lots of concern and considered as a promising technology for environmental decontamination. In this thesis, a novel kind of nonthermal plasma, namely gliding arc gas discharge, is utilized for the destruction of three kinds of AHOPs. Based on the knowledge of gliding arc physical characteristics, the destruction processes and mechanisms of Polycyclic Aromatic Hydrocarbons (PAHs),1,2-dicholorobenzene, polychlorinated dibenzo-p-dioxines (PCDDs) and polychlorinated dibenzofuran (PCDFs) are investigated. The main research contents are as followed:
1. Background introduction and literatures review. The treatment targets, PAHs, Chlorobenzenes and PCDD/Fs, are introduced from their chemical and physical properties and impactions to environment. And the decontamination methods are also reviewed. In addition, the definition, classification of plasma, generation methods of nonthermal plasma and its environmental applications are reviewed. Finally, the literatures and reports about gliding arc gas discharge are comprehensively reviewed from several aspects including its physical and chemical properties as well as its applications on environmental improvement, energy conversion and materials treatment.
2. Studies on physical properties of gliding arc plasma. Firstly, electrical characteristics of gliding arc at different operation condtions are investigated. Then, arc fluctuation is studied by analyzing arc voltage signals by using Fast Fourier Transform (FFT) method. Furthermore, main radical species in nitrogen, oxygen and air discharges were determined by means of optical emission spectroscopy. In this chapter, characteristics of an advanced type of gliding arc plasma:gliding arc in tornado (GAT) are also investigated. In order to study its electrical properties and fluctuation, arc voltage and current signals are measured at different experimental conditions. And the effect of gas input configuration on GAT physical properties is studied. Three working modes and the stable working mode of GAT are concluded based on the foregoing experimental results.
3. Studies on PAHs destruction by gliding arc plasma. Firstly, naphthalene is used as the target pollutant. The influence of external resistor of plasma generation circuit, gas type and naphthalene initial concentration on naphthalene destruction rate and process energy efficiency is investigated. The experiment results indicate that the destruction rate, which rises with increasing of concentration in carrier gas and decreasing of external resistance, can be achieved up to92.3%. The highest destruction process energy efficiency is3.6g/kWh which increases with rising external resistance. Secondly, the naphthalene destruction mechanism is proposed by analyzing all detected products. Finally, the simultaneous destruction process of four kinds of PAHs i.e. acenaphthene, fluorene, anthracene and pyrene is studied to increase the energy efficiency.
4. Studies on1,2-dichlorobenzene destruction by combined using gliding arc plasma and ozone. Firstly, the effect of key factors of experimental condition on1,2-dichlorobenzene destruction process is investigated and the results indicate that the destruction rate of1,2-dichlorobenzen can be achieved up to74.1%when external resistance is50kΩ and working gas is oxygen. The destruction main mechanisms in different carrier gas are proposed by analyzing gas products. Most of organic chlorine in1,2-dichlorobenzene is converted to inorganic chlorine, which is proved by study of chorine balance in destruction processes. In order to improve the gliding arc reactor performance for1,2-dichlorobenzene destruction, a novel method that combing gliding arc and ozone is utilized in this study. The effects of ozone injection place (in plasma area or in post-plasma area) and carrier gas type on the destruction process are studied. And the results indicate that the1,2-dichlorobenzene destruction process is enhanced significantly when the carrier gas is nitrogen or oxygen and ozone is injected in post-plasma area.
5. Studies on the destruction of PCDD/Fs in fly ash by using gliding arc in tornado. Solid waste fly ash is treated by GAT and its high concentration PCDD/Fs are destructed. The experimental results indicate that the mass destruction rate and I-TEQ destruction rate of PCDD/Fs can be achieved up to67.7%and72.3%, respectively, when oxygen is used as working gas. The I-TEQ concentrations of PCDD/Fs in the treated fly ash and in the off-gas are638pg-TEQ/g and342pg-TEQ/Nm3, respectively. Based on analysis of PCDD/Fs congeners distributions in original fly ash, treated fly ash and off-gas, two major PCDD/Fs destruction routes are proposed primarily:(1) PCDD/Fs are destructed by the direct interaction between GAT and fly ash surface;(2) PCDD/Fs are evaporated to gas phase and then destructed in the GAT by gas phase reactions.
(一)对研究相关背景和相关知识的文献综述。分别介绍了论文中的处理对象多环芳烃,氯苯和二恶英的基本物理化学性质,对环境的危害以及现有的处理方法。另外,对等离子体的定义和分类,非平衡等离子体的发生方式,以及非平衡等离子体技术在环境治理方面的应用进行了介绍。最后,对本文中所使用的滑动弧等离子技术的研究报道进行了充分综述,包括其物理化学特性,其在环境治理和能源转换,材料处理等方面的应用等。
(二)滑动弧等离子体的物理特性研究。分析滑动弧放电在不同工作条件下的电参数特性。并通过利用快速傅立叶变换方法分析电压信号获取等离子体的脉动的频率特性。利用光栅光谱仪检测了不同实验条件下的滑动弧放等离子体中的发射光谱,检测了在不同的气氛下,滑动弧产生的主要自由基,以及在反应器中自由基的轴向分布。另外,对新近发展龙旋风滑动弧反应器的工作特性进行了研究。分析了在不同实验工况下的电参数特性；研究了在不同流量配置下等离子体物理特性的变化,并基于以上分析总结了龙旋风滑动弧等离子体反应器的三种工作模式,找到了稳定的工作模式。
(三)利用滑动弧等离子体降解多环芳烃的研究。首先以萘为降解对象,研究了等离子体发生电路外部电阻、载气种类和萘的初始浓度对降解过程的影响。结果表明萘的降解率最高可达92.3%。降解率随着氧气浓度的增加而增加,随着外部电阻减小而增加。能量效率最高可达3.6g/kWh。降解能量效率随着外部电阻增大而明显增大。另外,检测了在不同气氛放电中的降解产物,通过分析降解产物分析萘在不同气氛放电中降解的主要机理。为了提高处理多环芳烃过程的能量效率,本文还研究了利用滑动弧同时脱除多种多环芳烃(二氢苊、芴、蒽和芘)过程。
(四)臭氧辅助滑动弧等离子体降解1,2-二氯苯的研究。分析滑动弧等离子体工作条件中的关键参数对1,2-二氯苯降解过程的影响。结果表明,1,2-二氯苯的降解率相对偏低,当外部电阻为50kΩ,载气为氧气时,降解率最高可达74.1%。通过检测在不同气氛下的主要降解产物,研究1,2-二氯苯的降解机理。为了提高1,2-二氯苯的降解率,本文利用臭氧辅助滑动弧对1,2-二氯苯进行降解。研究了臭氧在等离子体区域和后等离子体区域的作用以及气氛对这种新方法的影响。结果表明,只有在氮气和氧气等离子体放电下,在后等离子体区域同入臭氧才能够提高1,2-二氯苯的降解率。
(五)利用龙旋风滑动弧反应器降解垃圾焚烧飞灰中二恶英的研究。当载气为氧气时,飞灰中二恶英的降解率达到最高,二恶英的质量降解率为67.7%,毒性当量降解率为72.3%,降解后飞灰中的二恶英浓度为638pg-TEQ/g,尾气中二恶英的浓度为342pg-TEQ/Nm3。通过分析处理前后飞灰和尾气中二恶英同系物的分布以及飞灰表面形态变化,初步提出飞灰中二恶英的降解途径：一是等离子体直接作用于飞灰表面,实现二恶英的降解。二是飞灰中二恶英挥发之气相中,通过与等离子体中的高活性基团发生气相反应,实现降解的过程。
With the development of industry and improvement of life quality, release of kinds of pollutants to the environment is inevitable, which results in threats to the whole environment. Among of them, pollutions by Aromatic Hydrocarbon Organic Pollutants (AHOPs) are very serous. Scientists dedicate to invent and develop different technologies to control AHOPs emission. Compared with traditional methods, nonthermal plasma has some unique advantages that providing numerous free radicals and energetic electrons, low gas temperature and so on. Therefore, nonthermal plasma is received lots of concern and considered as a promising technology for environmental decontamination. In this thesis, a novel kind of nonthermal plasma, namely gliding arc gas discharge, is utilized for the destruction of three kinds of AHOPs. Based on the knowledge of gliding arc physical characteristics, the destruction processes and mechanisms of Polycyclic Aromatic Hydrocarbons (PAHs),1,2-dicholorobenzene, polychlorinated dibenzo-p-dioxines (PCDDs) and polychlorinated dibenzofuran (PCDFs) are investigated. The main research contents are as followed:
1. Background introduction and literatures review. The treatment targets, PAHs, Chlorobenzenes and PCDD/Fs, are introduced from their chemical and physical properties and impactions to environment. And the decontamination methods are also reviewed. In addition, the definition, classification of plasma, generation methods of nonthermal plasma and its environmental applications are reviewed. Finally, the literatures and reports about gliding arc gas discharge are comprehensively reviewed from several aspects including its physical and chemical properties as well as its applications on environmental improvement, energy conversion and materials treatment.
2. Studies on physical properties of gliding arc plasma. Firstly, electrical characteristics of gliding arc at different operation condtions are investigated. Then, arc fluctuation is studied by analyzing arc voltage signals by using Fast Fourier Transform (FFT) method. Furthermore, main radical species in nitrogen, oxygen and air discharges were determined by means of optical emission spectroscopy. In this chapter, characteristics of an advanced type of gliding arc plasma:gliding arc in tornado (GAT) are also investigated. In order to study its electrical properties and fluctuation, arc voltage and current signals are measured at different experimental conditions. And the effect of gas input configuration on GAT physical properties is studied. Three working modes and the stable working mode of GAT are concluded based on the foregoing experimental results.
3. Studies on PAHs destruction by gliding arc plasma. Firstly, naphthalene is used as the target pollutant. The influence of external resistor of plasma generation circuit, gas type and naphthalene initial concentration on naphthalene destruction rate and process energy efficiency is investigated. The experiment results indicate that the destruction rate, which rises with increasing of concentration in carrier gas and decreasing of external resistance, can be achieved up to92.3%. The highest destruction process energy efficiency is3.6g/kWh which increases with rising external resistance. Secondly, the naphthalene destruction mechanism is proposed by analyzing all detected products. Finally, the simultaneous destruction process of four kinds of PAHs i.e. acenaphthene, fluorene, anthracene and pyrene is studied to increase the energy efficiency.
4. Studies on1,2-dichlorobenzene destruction by combined using gliding arc plasma and ozone. Firstly, the effect of key factors of experimental condition on1,2-dichlorobenzene destruction process is investigated and the results indicate that the destruction rate of1,2-dichlorobenzen can be achieved up to74.1%when external resistance is50kΩ and working gas is oxygen. The destruction main mechanisms in different carrier gas are proposed by analyzing gas products. Most of organic chlorine in1,2-dichlorobenzene is converted to inorganic chlorine, which is proved by study of chorine balance in destruction processes. In order to improve the gliding arc reactor performance for1,2-dichlorobenzene destruction, a novel method that combing gliding arc and ozone is utilized in this study. The effects of ozone injection place (in plasma area or in post-plasma area) and carrier gas type on the destruction process are studied. And the results indicate that the1,2-dichlorobenzene destruction process is enhanced significantly when the carrier gas is nitrogen or oxygen and ozone is injected in post-plasma area.
5. Studies on the destruction of PCDD/Fs in fly ash by using gliding arc in tornado. Solid waste fly ash is treated by GAT and its high concentration PCDD/Fs are destructed. The experimental results indicate that the mass destruction rate and I-TEQ destruction rate of PCDD/Fs can be achieved up to67.7%and72.3%, respectively, when oxygen is used as working gas. The I-TEQ concentrations of PCDD/Fs in the treated fly ash and in the off-gas are638pg-TEQ/g and342pg-TEQ/Nm3, respectively. Based on analysis of PCDD/Fs congeners distributions in original fly ash, treated fly ash and off-gas, two major PCDD/Fs destruction routes are proposed primarily:(1) PCDD/Fs are destructed by the direct interaction between GAT and fly ash surface;(2) PCDD/Fs are evaporated to gas phase and then destructed in the GAT by gas phase reactions.
引文
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