大气压介质阻挡放电多针—同轴反应器结构优化及降解甲醛试验研究
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摘要
介质阻挡放电可以在常温大气压下产生低温等离子体，能耗低，且不需要昂贵的真空设备，特别适合于低温等离子体的工业化应用。大气压介质阻挡放电处理挥发性有机污染物是一种新型气态污染物治理技术，因其效率高、无选择性、使用范围广，近年来呈现出良好的应用前景。反应器电极结构是影响介质阻挡放电降解气态污染物效率的重要因素，因此优化反应器电极结构参数及其与电源参数的匹配对于提高气态污染物降解效率、降低能耗和介质阻挡放电大规模工业应用有重要的意义。
为降低起始放电电压和运行电压、提高电子密度和污染物降解效率，本文首先构建多针－同轴结构电晕介质阻挡放电反应器，试验检测放电特性，结果表明其放电模式是细丝（流注）模式。根据气体放电理论，每个放电细丝在交流电压的一个周期内可以划分为三个阶段进行分析研究：放电的形成——放电的击穿；放电击穿后，电流细丝流过气隙并传输电荷；在微放电通道中原子、分子的激发和反应动力学的启动。基于此，本文的主要研究内容和创新性成果有：
①在检测并分析大气压空气中多针－同轴反应器电晕介质阻挡放电特性的基础上，建立基于有限元的电准静态空间电场分布计算模型，研究电极结构参数对反应器空间电场分布的影响；以大气压空气中不均匀场电子雪崩产生临界电场强度为判据，采用电准静态模型首次优化多针－同轴电极结构参数，并以试验验证。
仿真结果还表明，相邻针之间相互作用显著影响反应器空间电场分布，所以本文进一步采用流注放电流体力学模型首次模拟相邻针相互作用对大气压空气中多针流注放电发展的影响：通过对比分析单针与多针流注放电过程中电场强度、电子和正离子数密度随时空发展过程，以及电子平均能量分布，表明多针流注的发展速度、流注发展轴线上电场强度、电子平均能量分布以及电子数密度和正离子数密度均比单针流注的小。但是，在相邻针相互作用下，多针结构的电晕放电性质较单针结构减弱，且反应器内非流注区域电场强度和电子平均能量能保持比单针结构大的水平，这对于降解气态有机污染物等DBD工业应用是有利的。
②正交试验研究周期传输电荷量最大的多针－同轴电极结构参数与电源参数的配合，方差分析结果表明试验因素对目标因素周期传输电荷量影响的显著性排序是电压幅值>频率>针间距>针长>相邻针夹角，长度3.5mm和2mm的针以纵向相邻针角度为45°间隔2.5mm排列的电极结构与电源频率21kHz的匹配令目标因素最大。
③正交试验研究甲醛降解率最高的电极结构参数与电源参数的匹配，结果与目标因素为周期传输电荷量的正交试验结果相同；借助分子模拟软件，首次采用密度泛函理论研究介质阻挡放电降解甲醛的机理：建立化学反应相对能计算模型，模型中考虑常压常温条件下的热力学焓校正值；设计介质阻挡放电降解甲醛过程中可能的主要自由基反应过程和自由基生成路径，并进行细致分析；最后将本文研究成果与文献研究成果对比分析，说明密度泛函理论研究可以作为试验研究的有效可靠补充手段。
Dielectric barrier discharge (DBD) can produce large volume and high-energy-density non-thermal plasma (NTP) at atmospheric pressure over a wide range offrequencies without expensive vacuum equipment, so it has a number of industrialapplications, such as surface modification, environmental protection, medicine, andplasma displays. Gaseous organic pollutant removal through DBD is a new techniquethat has appeared promising application prospect because of high efficiency andnon-selectivity. Reactor configuration has a major effect on DBD characteristics andpollutant removal efficiency, thus reactor configuration optimization and the match ofthe DBD reactor structure and the power supply is of great significance for large-scaleindustrial application of DBD.
To decrease initial discharge voltage and operating voltage, increase electrondensity and pollutant removal efficiency, multineedle-to-cylinder (MC) corona-DBDreactor is designed at first in this thesis. Experimental discharge currents and imagesshow the discharge pattern at atmospheric air is filament (streamer). According todischarge theory, the life cycle of one such filament can be discerned three separate steps:the formation of the avalanche, i.e., the electrical breakdown; the ensuing current pulse ortransport of charge across the gap; and simultaneously the excitation of the atoms andmolecules present and thus initiation of the reaction kinetics. Researches have been madeaiming at the three separate steps of the filament:
①Based on the quasi-static maxwell equation, a quasi-static field model ispresented to calculate the electric field distribution in the reactor using finite-elementmethod. The critical electric field strength of avalanche production is adopted as thecriterion to optimize the structure and parameters of MC reactor, which is validated byfurther experiments.
Simulation results also show that mutual effect among adjacent needles influenceDBD characteristics. Therefore, the fluid-hydrodynamic model is employed toinvestigate the the influence of the mutual effect on the multi-needle streamerpropagation. The comparison and analysis between the electric field, electrons andpositive ions number density, electron average energy of streamer discharge insingle-needle geometry (SNG) and three-needle geometry (TNG) show that the averagepropagation velocities, electric fields distribution, electron average energy, the electron density along the streamer propagation axis in TNG decreas compared with those in theSNG. However, the corona character is weakened in TNG. Meanwhile, the electric field,electrons and the electron average energies out of streamer domain in TNG are greaterthan those in SNG, which is favorable to gasous pollutant removal.
②The matching of electrode configuration and power supply parameters is studiedby orthogonal design in combination with Lissajous figures, in which the value oftransported charges per cycle is adopthe as the goal factor. The results of the varianceanalysis interpret that the influence of Upis the most remarkable. The next influencingfactor is f while NL and INRA do not affect the charges transferred remarkably. Theoptimal experiment plan is f=21kHz, and NL is3.5mm and2mm alternatively spacedwith INRA of45°. Orthogonal experiment results are experimentally validated byfurther experiments involved with all NL and INRA combinations.
③The orthogonal experiment is used to optimize the matching between MCstructure and the power supply to achieve the highest removal efficiency. Densityfunctional theory (DFT) is used to study the pathways of formaldehyde removal underDBDs plasma conditions through molecular simulation package. The calculation modelof the relative energy of the reactions is defined, in which adjustment term concerningthe actual experiment conditions is considered. Possible radical reactions and theformation reactions of radicals are designed and investigated with DFT. The previouslycorrelative theoretical or experimental results are also included in this work.Comparative results between the previous investigation and the present workdemonstrate that theoretical calculation with DFT is an efficient and reliable supplementfor experimental research.
为降低起始放电电压和运行电压、提高电子密度和污染物降解效率，本文首先构建多针－同轴结构电晕介质阻挡放电反应器，试验检测放电特性，结果表明其放电模式是细丝（流注）模式。根据气体放电理论，每个放电细丝在交流电压的一个周期内可以划分为三个阶段进行分析研究：放电的形成——放电的击穿；放电击穿后，电流细丝流过气隙并传输电荷；在微放电通道中原子、分子的激发和反应动力学的启动。基于此，本文的主要研究内容和创新性成果有：
①在检测并分析大气压空气中多针－同轴反应器电晕介质阻挡放电特性的基础上，建立基于有限元的电准静态空间电场分布计算模型，研究电极结构参数对反应器空间电场分布的影响；以大气压空气中不均匀场电子雪崩产生临界电场强度为判据，采用电准静态模型首次优化多针－同轴电极结构参数，并以试验验证。
仿真结果还表明，相邻针之间相互作用显著影响反应器空间电场分布，所以本文进一步采用流注放电流体力学模型首次模拟相邻针相互作用对大气压空气中多针流注放电发展的影响：通过对比分析单针与多针流注放电过程中电场强度、电子和正离子数密度随时空发展过程，以及电子平均能量分布，表明多针流注的发展速度、流注发展轴线上电场强度、电子平均能量分布以及电子数密度和正离子数密度均比单针流注的小。但是，在相邻针相互作用下，多针结构的电晕放电性质较单针结构减弱，且反应器内非流注区域电场强度和电子平均能量能保持比单针结构大的水平，这对于降解气态有机污染物等DBD工业应用是有利的。
②正交试验研究周期传输电荷量最大的多针－同轴电极结构参数与电源参数的配合，方差分析结果表明试验因素对目标因素周期传输电荷量影响的显著性排序是电压幅值>频率>针间距>针长>相邻针夹角，长度3.5mm和2mm的针以纵向相邻针角度为45°间隔2.5mm排列的电极结构与电源频率21kHz的匹配令目标因素最大。
③正交试验研究甲醛降解率最高的电极结构参数与电源参数的匹配，结果与目标因素为周期传输电荷量的正交试验结果相同；借助分子模拟软件，首次采用密度泛函理论研究介质阻挡放电降解甲醛的机理：建立化学反应相对能计算模型，模型中考虑常压常温条件下的热力学焓校正值；设计介质阻挡放电降解甲醛过程中可能的主要自由基反应过程和自由基生成路径，并进行细致分析；最后将本文研究成果与文献研究成果对比分析，说明密度泛函理论研究可以作为试验研究的有效可靠补充手段。
Dielectric barrier discharge (DBD) can produce large volume and high-energy-density non-thermal plasma (NTP) at atmospheric pressure over a wide range offrequencies without expensive vacuum equipment, so it has a number of industrialapplications, such as surface modification, environmental protection, medicine, andplasma displays. Gaseous organic pollutant removal through DBD is a new techniquethat has appeared promising application prospect because of high efficiency andnon-selectivity. Reactor configuration has a major effect on DBD characteristics andpollutant removal efficiency, thus reactor configuration optimization and the match ofthe DBD reactor structure and the power supply is of great significance for large-scaleindustrial application of DBD.
To decrease initial discharge voltage and operating voltage, increase electrondensity and pollutant removal efficiency, multineedle-to-cylinder (MC) corona-DBDreactor is designed at first in this thesis. Experimental discharge currents and imagesshow the discharge pattern at atmospheric air is filament (streamer). According todischarge theory, the life cycle of one such filament can be discerned three separate steps:the formation of the avalanche, i.e., the electrical breakdown; the ensuing current pulse ortransport of charge across the gap; and simultaneously the excitation of the atoms andmolecules present and thus initiation of the reaction kinetics. Researches have been madeaiming at the three separate steps of the filament:
①Based on the quasi-static maxwell equation, a quasi-static field model ispresented to calculate the electric field distribution in the reactor using finite-elementmethod. The critical electric field strength of avalanche production is adopted as thecriterion to optimize the structure and parameters of MC reactor, which is validated byfurther experiments.
Simulation results also show that mutual effect among adjacent needles influenceDBD characteristics. Therefore, the fluid-hydrodynamic model is employed toinvestigate the the influence of the mutual effect on the multi-needle streamerpropagation. The comparison and analysis between the electric field, electrons andpositive ions number density, electron average energy of streamer discharge insingle-needle geometry (SNG) and three-needle geometry (TNG) show that the averagepropagation velocities, electric fields distribution, electron average energy, the electron density along the streamer propagation axis in TNG decreas compared with those in theSNG. However, the corona character is weakened in TNG. Meanwhile, the electric field,electrons and the electron average energies out of streamer domain in TNG are greaterthan those in SNG, which is favorable to gasous pollutant removal.
②The matching of electrode configuration and power supply parameters is studiedby orthogonal design in combination with Lissajous figures, in which the value oftransported charges per cycle is adopthe as the goal factor. The results of the varianceanalysis interpret that the influence of Upis the most remarkable. The next influencingfactor is f while NL and INRA do not affect the charges transferred remarkably. Theoptimal experiment plan is f=21kHz, and NL is3.5mm and2mm alternatively spacedwith INRA of45°. Orthogonal experiment results are experimentally validated byfurther experiments involved with all NL and INRA combinations.
③The orthogonal experiment is used to optimize the matching between MCstructure and the power supply to achieve the highest removal efficiency. Densityfunctional theory (DFT) is used to study the pathways of formaldehyde removal underDBDs plasma conditions through molecular simulation package. The calculation modelof the relative energy of the reactions is defined, in which adjustment term concerningthe actual experiment conditions is considered. Possible radical reactions and theformation reactions of radicals are designed and investigated with DFT. The previouslycorrelative theoretical or experimental results are also included in this work.Comparative results between the previous investigation and the present workdemonstrate that theoretical calculation with DFT is an efficient and reliable supplementfor experimental research.
引文
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