介质阻挡放电低温等离子体降解亚甲基蓝溶液及其体系气液相中活性粒子化学行为分析
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摘要
本文针对色度深、毒性大的有机废水，以亚甲基蓝溶液作为实验研究对象，采用介质阻挡放电（DBD）等离子体技术对其进行降解实验研究，对降解过程气、液相中的活性粒子的化学行为进行探索。
主要完成的内容为：
（1）分析空气气氛条件下DBD等离子体对亚甲基蓝溶液的降解效果。对DBD等离子体降解亚甲基蓝溶液的中间产物和最终产物进行了检测，推测了亚甲基蓝分子的降解反应历程。考察了以氩气、空气和氢气作为放电气氛条件下，DBD等离子体降解亚甲基蓝溶液的效果，分析了不同放电气氛对DBD等离子体降解亚甲基蓝溶液过程的影响机理。通过对DBD体系液相的设计，初步探索了降解反应在DBD体系中发生的位置。实验结果表明：以空气为放电气氛时，亚甲基蓝溶液有最高的降解率，放电30min时，亚甲基蓝溶液降解率为84.8%。分别以氩气、空气和氢气作为DBD过程放电气氛，对比了亚甲基蓝溶液的pH值、电导率和总有机碳含量（TOC）的变化趋势及变化幅度。在对实验结果进行综合分析的基础上，探讨了不同的放电气氛对DBD等离子体降解亚甲基蓝溶液过程的影响机理：在不同的放电气氛条件下，DBD过程产生的气相活性粒子的种类、气相活性粒子的能量状态以及放电过程气相中产生的一些特殊放电产物，是影响DBD等离子体降解亚甲基蓝溶液过程的重要因素。通过实验设计对DBD体系中降解反应发生位置进行初步探索，实验结果表明DBD体系中降解反应不仅仅发生在气液接触面，而是在整个液相区域均有发生。
（2）采用Optical Emission Spectroscopy （OES）检测方法，对以氩气、空气和氢气作为放电气氛的DBD过程气相中的活性粒子进行检测分析。分别考察了在三种不同的放电气氛条件下，DBD过程气相中产生的主要激发态分子（原子）的种类及其能量状态。采用Boltzmann-Plot方法计算了以氩气作为放电气氛的DBD过程的电子激发温度，并考察了输入电压和电源频率对电子激发温度的影响情况。对以空气为放电气氛的DBD过程产生的主要激发态氮分子（原子）、主要激发态氧分子（原子）以及放电过程中产生的氮氧化物和臭氧进行了分析。
（3）考察了不同的放电气氛条件对DBD过程液相中羟基自由基和过氧化氢浓度的影响。通过添加不同的猝灭剂，分别对DBD降解亚甲基蓝溶液过程中产生的羟基自由基和过氧化氢进行屏蔽，依次考察了羟基自由基和过氧化氢对亚甲基蓝溶液降解过程的贡献。实验结果表明：在以空气作为DBD过程的放电气氛时，液相中产生的羟基自由基浓度最高。放电30min时，液相中羟基自由基的浓度为2.27×10-4mol/L。当以氩气作为DBD过程放电气氛的条件下，液相中产生的过氧化氢浓度最高，放电30min时，液相中过氧化氢的浓度为1.27×10-5（w/w）。以氢气作为DBD过程放电气氛的条件下，液相中产生的过氧化氢和羟基自由基浓度均最低，放电30min，羟基自由基和过氧化氢的浓度分别为6.05×10-5mol/L和2.32×10-6（w/w）。添加猝灭剂的屏蔽实验结果表明，分别在以氩气、空气和氢气为放电气氛条件下，放电30min时，羟基自由基和过氧化氢对亚甲基蓝降解过程的贡献值依次为47.8%和21.8%、29.0%和18.8%以及44.4%和16.6%。
（4）揭示了DBD等离子体降解亚甲基蓝溶液的作用过程机理。其作用过程分为以下三个阶段：
第一阶段：气相激发、离解和电离阶段，即气相中激发态活性粒子和高能电子的产生阶段。
第二阶段：气相中激发态活性粒子和高能电子与液相水分子的作用过程，同时也是液相中活性粒子（羟基自由基和过氧化氢等）的产生阶段。即液相中的羟基自由基和过氧化氢等活性粒子是液相中水分子与气相中激发态活性粒子和高能电子发生相互作用的产物。
第三阶段：液相中活性粒子（羟基自由基和过氧化氢等）与亚甲基蓝分子的作用阶段。
This essay is focused on the degradation of the high toxic organic wastewater with darkcolor. Methylene blue solution was used as the research subject. Dielectric Barrier Discharge(DBD) plasma was employed to treat methylene blue solution and the treatment process wasstudied in detail. The radical species in the gas phase and the liquid phase of the DBDdegradation process were studied.
The main contents are shown as below:
(1) Took air as the working gas of the DBD process, the intermediate products and thefinal products in the methylene blue degradation process by DBD plasma were detected. Thedegradation path of the methylene blue molecule was inferred based on the analysis of themolecular structure. The degradation effect of methylene blue solution was studied whenhydrogen, argon or air was employed as the different working gas of the DBD process,respectively. The liquid phase in the DBD system was designed to analyze the occurringposition of the degradation reactions. The results indicate that: the degradation percentage ofmethylene blue solution reached the maximum value when air was used as the working gasand the degradation percentage of methylene blue solution was84.8%when it was treated for30min. when different working gases were employed, the variation trends and scales of thepH value, Total Organic Carbon (TOC) value and conductivity during the DBD processeswere studied. The influence mechanism of the working gas on the DBD degradation processwas inferred as that: different radical species were generated when different working gaseswere employed as the working gases of the DBD processes. The main reason caused thedifferent degradation effect was that different radical species and discharge products weregenerated when different working gases were employed. The experimental results alsoindicate that the degradation reactions occurred not only at the interface of the gas-liqud phase,but in the entire liquid phase of the DBD system.
(2) The radical species generated in the gas phase during the three different DBDprocesses were studied using Optical Emission Spectroscopy (OES) method. The energybalance of the DBD process was studied when different working gas was employed. Thespecies of the radical and their energy states were analyzed when argon, hydrogen or air wasemployed as the working gas, respectively. Boltzman-plot method was used to calculate theelectron temperature when argon was employed as the working gas of the DBD process. Thedischarge products (ozone and nitrogen oxidize) were quantitatively detected when air wasemployed as the working gas of the DBD process.
(3) Hydroxyl radical and hydrogen peroxide in the liquid phase were quantitativelydetermined. Different quenchers were added into methylene blue solution to analyze thecontributions of the hydroxyl radical and hydrogen peroxide to the methylene bluedegradation process, respectively. The results indicate that: when air was employed as theworking gas of the DBD process, the concentration of hydroxyl radical in the liquid phasereached the maximum value. When air was employed as the working gas, the concentratio n ofhydroxyl radical in the liquid phase was2.27×10-4mol/L when it was treated for30min.When argon was employed as the working gas, the concentration of hydrogen peroxide in theliquid phase reached the maximum value. When argon was employed as the working gas, theconcentration of hydrogen peroxide in the liquid phase was1.27×10-5(w/w) when it wastreated for30min. When hydrogen was employed as the working gas of the DBD process, theconcentrations of hydrogen peroxide and hydroxyl radical were both the lowest and they were6.05×10-5mol/L and2.32×10-6(w/w) when it was treated for30min. When argon, air orhydrogen was employed as the working gas, the contribution values of hydroxyl radical andhydrogen peroxide were47.8%and21.8%,29.0%and18.8%,44.4%and16.6%,respectively.
(4) It was suggested that the methylene blue solution DBD degradation process wasdivided into three stages:
The first stage: the excitation, dissociation and ionization process in the gas phase. It wasalso the generation processes of the radical species and high energy electrons in the gas phase;
The second stage: the interaction process between the radical species and the watermolecules at the gas-liquid interface. It was also the radical species (hydroxyl radical,hydrogen peroxide et al.) generation process in the liquid phase. Hydroxyl radical andhydrogen peroxide are the products of the interactions between radical species, high energyelectrons and the water molecules.
The third stage: the reaction processes between radical species (hydroxyl radical,hydrogen peroxide et al.) and methylene blue molecules in the liquid phase.
主要完成的内容为：
（1）分析空气气氛条件下DBD等离子体对亚甲基蓝溶液的降解效果。对DBD等离子体降解亚甲基蓝溶液的中间产物和最终产物进行了检测，推测了亚甲基蓝分子的降解反应历程。考察了以氩气、空气和氢气作为放电气氛条件下，DBD等离子体降解亚甲基蓝溶液的效果，分析了不同放电气氛对DBD等离子体降解亚甲基蓝溶液过程的影响机理。通过对DBD体系液相的设计，初步探索了降解反应在DBD体系中发生的位置。实验结果表明：以空气为放电气氛时，亚甲基蓝溶液有最高的降解率，放电30min时，亚甲基蓝溶液降解率为84.8%。分别以氩气、空气和氢气作为DBD过程放电气氛，对比了亚甲基蓝溶液的pH值、电导率和总有机碳含量（TOC）的变化趋势及变化幅度。在对实验结果进行综合分析的基础上，探讨了不同的放电气氛对DBD等离子体降解亚甲基蓝溶液过程的影响机理：在不同的放电气氛条件下，DBD过程产生的气相活性粒子的种类、气相活性粒子的能量状态以及放电过程气相中产生的一些特殊放电产物，是影响DBD等离子体降解亚甲基蓝溶液过程的重要因素。通过实验设计对DBD体系中降解反应发生位置进行初步探索，实验结果表明DBD体系中降解反应不仅仅发生在气液接触面，而是在整个液相区域均有发生。
（2）采用Optical Emission Spectroscopy （OES）检测方法，对以氩气、空气和氢气作为放电气氛的DBD过程气相中的活性粒子进行检测分析。分别考察了在三种不同的放电气氛条件下，DBD过程气相中产生的主要激发态分子（原子）的种类及其能量状态。采用Boltzmann-Plot方法计算了以氩气作为放电气氛的DBD过程的电子激发温度，并考察了输入电压和电源频率对电子激发温度的影响情况。对以空气为放电气氛的DBD过程产生的主要激发态氮分子（原子）、主要激发态氧分子（原子）以及放电过程中产生的氮氧化物和臭氧进行了分析。
（3）考察了不同的放电气氛条件对DBD过程液相中羟基自由基和过氧化氢浓度的影响。通过添加不同的猝灭剂，分别对DBD降解亚甲基蓝溶液过程中产生的羟基自由基和过氧化氢进行屏蔽，依次考察了羟基自由基和过氧化氢对亚甲基蓝溶液降解过程的贡献。实验结果表明：在以空气作为DBD过程的放电气氛时，液相中产生的羟基自由基浓度最高。放电30min时，液相中羟基自由基的浓度为2.27×10-4mol/L。当以氩气作为DBD过程放电气氛的条件下，液相中产生的过氧化氢浓度最高，放电30min时，液相中过氧化氢的浓度为1.27×10-5（w/w）。以氢气作为DBD过程放电气氛的条件下，液相中产生的过氧化氢和羟基自由基浓度均最低，放电30min，羟基自由基和过氧化氢的浓度分别为6.05×10-5mol/L和2.32×10-6（w/w）。添加猝灭剂的屏蔽实验结果表明，分别在以氩气、空气和氢气为放电气氛条件下，放电30min时，羟基自由基和过氧化氢对亚甲基蓝降解过程的贡献值依次为47.8%和21.8%、29.0%和18.8%以及44.4%和16.6%。
（4）揭示了DBD等离子体降解亚甲基蓝溶液的作用过程机理。其作用过程分为以下三个阶段：
第一阶段：气相激发、离解和电离阶段，即气相中激发态活性粒子和高能电子的产生阶段。
第二阶段：气相中激发态活性粒子和高能电子与液相水分子的作用过程，同时也是液相中活性粒子（羟基自由基和过氧化氢等）的产生阶段。即液相中的羟基自由基和过氧化氢等活性粒子是液相中水分子与气相中激发态活性粒子和高能电子发生相互作用的产物。
第三阶段：液相中活性粒子（羟基自由基和过氧化氢等）与亚甲基蓝分子的作用阶段。
This essay is focused on the degradation of the high toxic organic wastewater with darkcolor. Methylene blue solution was used as the research subject. Dielectric Barrier Discharge(DBD) plasma was employed to treat methylene blue solution and the treatment process wasstudied in detail. The radical species in the gas phase and the liquid phase of the DBDdegradation process were studied.
The main contents are shown as below:
(1) Took air as the working gas of the DBD process, the intermediate products and thefinal products in the methylene blue degradation process by DBD plasma were detected. Thedegradation path of the methylene blue molecule was inferred based on the analysis of themolecular structure. The degradation effect of methylene blue solution was studied whenhydrogen, argon or air was employed as the different working gas of the DBD process,respectively. The liquid phase in the DBD system was designed to analyze the occurringposition of the degradation reactions. The results indicate that: the degradation percentage ofmethylene blue solution reached the maximum value when air was used as the working gasand the degradation percentage of methylene blue solution was84.8%when it was treated for30min. when different working gases were employed, the variation trends and scales of thepH value, Total Organic Carbon (TOC) value and conductivity during the DBD processeswere studied. The influence mechanism of the working gas on the DBD degradation processwas inferred as that: different radical species were generated when different working gaseswere employed as the working gases of the DBD processes. The main reason caused thedifferent degradation effect was that different radical species and discharge products weregenerated when different working gases were employed. The experimental results alsoindicate that the degradation reactions occurred not only at the interface of the gas-liqud phase,but in the entire liquid phase of the DBD system.
(2) The radical species generated in the gas phase during the three different DBDprocesses were studied using Optical Emission Spectroscopy (OES) method. The energybalance of the DBD process was studied when different working gas was employed. Thespecies of the radical and their energy states were analyzed when argon, hydrogen or air wasemployed as the working gas, respectively. Boltzman-plot method was used to calculate theelectron temperature when argon was employed as the working gas of the DBD process. Thedischarge products (ozone and nitrogen oxidize) were quantitatively detected when air wasemployed as the working gas of the DBD process.
(3) Hydroxyl radical and hydrogen peroxide in the liquid phase were quantitativelydetermined. Different quenchers were added into methylene blue solution to analyze thecontributions of the hydroxyl radical and hydrogen peroxide to the methylene bluedegradation process, respectively. The results indicate that: when air was employed as theworking gas of the DBD process, the concentration of hydroxyl radical in the liquid phasereached the maximum value. When air was employed as the working gas, the concentratio n ofhydroxyl radical in the liquid phase was2.27×10-4mol/L when it was treated for30min.When argon was employed as the working gas, the concentration of hydrogen peroxide in theliquid phase reached the maximum value. When argon was employed as the working gas, theconcentration of hydrogen peroxide in the liquid phase was1.27×10-5(w/w) when it wastreated for30min. When hydrogen was employed as the working gas of the DBD process, theconcentrations of hydrogen peroxide and hydroxyl radical were both the lowest and they were6.05×10-5mol/L and2.32×10-6(w/w) when it was treated for30min. When argon, air orhydrogen was employed as the working gas, the contribution values of hydroxyl radical andhydrogen peroxide were47.8%and21.8%,29.0%and18.8%,44.4%and16.6%,respectively.
(4) It was suggested that the methylene blue solution DBD degradation process wasdivided into three stages:
The first stage: the excitation, dissociation and ionization process in the gas phase. It wasalso the generation processes of the radical species and high energy electrons in the gas phase;
The second stage: the interaction process between the radical species and the watermolecules at the gas-liquid interface. It was also the radical species (hydroxyl radical,hydrogen peroxide et al.) generation process in the liquid phase. Hydroxyl radical andhydrogen peroxide are the products of the interactions between radical species, high energyelectrons and the water molecules.
The third stage: the reaction processes between radical species (hydroxyl radical,hydrogen peroxide et al.) and methylene blue molecules in the liquid phase.
引文
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