介质阻挡放电降解甲基紫废水及尾气中NO_x的光谱分析及机理研究
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摘要
随着世界经济和社会的快速发展,环境污染问题也日益严重,各种污染物对人类的生存环境及人身健康带来严重影响,因此各国都在制定越来越严格的排放标准。目前我国印染废水处理中普遍存在废水脱色困难的问题；在柴油发动机尾气的富氧条件下NOx的净化,依旧是研究者们面临的难题。
介质阻挡放电(DBD)等离子体作为一种富含高能活性粒子的物质,它的效率较高且无二次污染,是一种绿色环保处理技术。本论文中,作者研制了介质阻挡放电装置及配套电源,利用该装置对不同气体的放电特性及发射光谱进行了研究,并在甲基紫废水处理及柴油机尾气处理方面进行了相关研究。概括起来,在本论文的工作中,主要取得以下研究结果：
(1)自制介质阻挡放电装置及配套的电源,搭建了稳定的介质阻挡放电实验平台。
(2)分别对Ar、Ar+O2、He、He+O2、N2、N2+O2、O2及空气体系的放电特性及发射光谱进行了研究。结果表明,除了He气放电通常为准辉光放电外,其余气体放电均为丝状放电。在Ar及Ar+02气放电中,测到很强的N原子(寿命很短)谱线,在Ar气放电中测到很强的高反应活性的OH自由基的谱线,而在其它气体放电中未测到OH自由基的谱线,意味着Ar气放电可能更有利用价值。另外在N2、N2+02及空气放电中观察到了NO (A—X)的谱线,但在N2+02及空气放电中该谱线强度要弱很多,而且在O2气放电中未测到NO (A—X),因为氧气含量较高时NO与02、O3或O原子继续反应生成NO2而被减少,且随氧气含量的增加而迅速减少。
(3)对甲基紫脱色处理结果表明,甲基紫溶液脱色率由高到低依次为O2>He+O2>He,且He+O2混合气和单纯02气放电下的脱色率相差不大。He气放电消耗的能量密度低,但脱色率小于50%；O2气放电处理甲基紫溶液脱色率达99.5%,但是消耗的能量密度高达32.5kJ/L; He+O2混合气放电处理甲基紫溶液体现了很好的脱色效果同时能量消耗较低,处理180s时脱色率达96%而能量消耗却只有7.7kJ／L。因此提出He+02混合气为最佳用于甲基紫溶液脱色的放电气体组合,既能取得高脱色率又能降低能耗。
对甲基紫的降解机理分析得出,OH基和02对甲基紫的降解起着关键作用,而OH基主要通过与氧有关的反应获得,因此与活性氧的含量有关。因此认为活性氧(如O2-·、H2O2、OH、O等)是甲基紫脱色的关键粒子。
(4)利用自制的DBD装置结合选择催化还原(SCR)装置建立了多功能的DBD协同SCR脱除NOx研究平台。分别以C2H5OH和C3H6为还原剂、以Ag/Al2O3为催化剂,研究了高NOx浓度(800ppm左右)及高空速(50000h-1)下,DBD等离子体协同SCR脱除NOx的特性及反应机理,同时考察了尾气温度对NOx脱除的影响,并重点研究了150℃低温时的NOx脱除特性,及利用]FTIR光谱分析了反应产物。
DBD等离子体协同SCR作用在低温时取得了很好的脱除效果。C2H5OH为还原剂,在含8%H2O且温度150℃的模拟柴油机尾气中NOx脱除率高达80%,其中NO脱除率高达90%。C3H6为还原剂,尾气中不含水时NOx脱除率最高达88%,NO脱除率高达94%,但加入8%H2O后NOx脱除率降低至60%。对FTIR吸收光谱的分析进一步确认了SCR单独作用在低温时对NOx脱除无效,而DBD协同SCR却能有效脱除NOx,同时也脱除了碳氢,NOx及碳氢脱除后的最终产物主要为N2、C02和H2O。
通过对比研究DBD和SCR分别作用及协同作用时的NOx脱除特性,提出NOx脱除机理为：放电形成时等离子体中的强氧化性粒子与碳氢作用生成的有机活性基团(主要为CH3O2)在催化剂促进下迅速将NO氧化成NO2；随着电压升高,NO2在催化剂表面与碳氢作用生成活性中间产物CxHyNzO,NO2含量越高则生成的活性中间产物越多；放电在活化气体的同时也提高了催化床的温度,从而间接提高了催化剂的活性,最终NOx在催化剂促进下被CxHyNzO脱除,同时CxHyNzO被转化为CO2和H2O而脱除。实验证明了低温时等离子体中强氧化性粒子O3、HO2等对NO的作用很弱,而被DBD活化的碳氢才是NO有效氧化的关键粒子。
With the rapid development of economy and society in the world, the environmental pollution is increasingly serious and harmful to the human living environment and health, so various countries are formulating increasingly strict emission rule. Now, in our country it is commonly difficult for the decoloration of waste water and for the removal of NOx in diesel engine exhaust gases.
Dielectric Barrier Discharges (DBD) plasma which includes energetic electrons and active particles is effective and environmental techniques of handling. In this paper, the author developed DBD device and matched power supply source, whereby the characteristics and emission spectrums of various gases discharge were studied, and the related investigations were taken for the decoloration of waste water and the removal of NOx in diesel engine exhaust gases. In general, the achieved achievements were mainly as follows:
(1) The DBD device and its matched power supply source was developed, and by the device the research platform of DBD was build.
(2) The characteristics and emission spectrums of discharge in Ar, Ar+O2, He, He+02, N2, N2+O2, O2, and air were studied. Results show discharge is similar glow in He gas and filar in the others. The intense spectral line of N atom whose lifetime is short was observed in Ar and Ar+O2 discharge, and the reactive OH radical was observed in Ar discharge but not in the others, so it might be more value in application. Additionally, the spectral line of NO(A—X) was observed in N2, N2+O2, and air discharge, and the intensity of spectral line rapidly decreased with the increasing scale of O2 gas.
(3) The results of decoloration for methyl violet show that the decoloration ratio from high to low was O2, He+02 and He, and the effect was similar in He+O2 and O2 gas discharge. For He gas discharge, consumed energy density is low, but the decoloration ratio is also lower than 50%; for O2 gas discharge, the decoloration ratio of 99.5% was achieved, but the high energy density of 32.5kJ/L was required; for He+02 discharge, the decoloration ratio of 96% was achieved, but the consumed energy density was only 7.7kJ/L. So we propose that the mixed gases of He+02 are optimal for the decoloration of methyl violet, because the high decoloration ratio can be achieved and low energy density will be cost in the system.
By analyzing the decoloration mechanism of methyl violet, it is considered that OH radical and O2 gas play a key role in the decoloration, and OH radical is mainly got by the reactions related with O. So we consider the reactive oxygen (such as O2-·,H2O2, OH, O) as the key particles for the decoloration of methyl violet.
(4) Using the self-developed DBD device combined with selective catalytic reduction (SCR) device, we build a research platform of DBD cooperating with SCR for NOx removal. The characteristics of NOx removal and reaction mechanisms by DBD cooperated with SCR were investigated under the conditions of high NOx concentration (800 ppm) and high space velocity (50000 h-1). Meanwhile, the effect of temperature on NOx removal was also studied, especially the NOx removal at the low temperature of 150℃was investigated and the reaction products were analyzed by FTIR spectra.
By DBD cooperated with SCR the high NOx removal rate was achieved at low temperature. With C2H5OH as reductant, the NOx removal rate of 80% and the NO removal rate of 90% were achieved at 150℃when 8% H2O was fed into the exhaust gases. With C3H6 as reductant, the NOx removal rate of 88% and the NO removal rate of 94% were achieved at 150℃in dry gases, but the NOx removal rate decreased to 60% when 8% H2O was fed into the exhaust gases. The FTIR spectra confirm the NOx can effectively be removed by DBD cooperated with SCR, and the reaction products are mainly N2, CO2 and H2O.
By contrast research on DBD and SCR individually and together impacting on NOx removal, the reaction mechanism of NOx removal were proposed as follows:when discharge came into being, strong oxidative particles in plasma reacted with hydrocarbons to get organic reactive particles which rapidly oxidized NO to NO2 at the acceleration of catalyst; NO2 reacted with hydrocarbons to get CxHyNzO compound over catalysts, and the more NO2 the more CxHyNzO compound were produced; discharge resulted in the activation of hydrocarbons and the rise of catalyst bed temperature, so finally the NOx was removed by reaction with CxHyNzO over catalyst, and simultaneously the hydrocarbons were removed by the generation of CO2 and H2O.Experiments show the role of O3, HO2, and so on in plasma is weak in reaction with NO, and the hydrocarbons are just the key particles for the effective oxidation of NO to NO2.
介质阻挡放电(DBD)等离子体作为一种富含高能活性粒子的物质,它的效率较高且无二次污染,是一种绿色环保处理技术。本论文中,作者研制了介质阻挡放电装置及配套电源,利用该装置对不同气体的放电特性及发射光谱进行了研究,并在甲基紫废水处理及柴油机尾气处理方面进行了相关研究。概括起来,在本论文的工作中,主要取得以下研究结果：
(1)自制介质阻挡放电装置及配套的电源,搭建了稳定的介质阻挡放电实验平台。
(2)分别对Ar、Ar+O2、He、He+O2、N2、N2+O2、O2及空气体系的放电特性及发射光谱进行了研究。结果表明,除了He气放电通常为准辉光放电外,其余气体放电均为丝状放电。在Ar及Ar+02气放电中,测到很强的N原子(寿命很短)谱线,在Ar气放电中测到很强的高反应活性的OH自由基的谱线,而在其它气体放电中未测到OH自由基的谱线,意味着Ar气放电可能更有利用价值。另外在N2、N2+02及空气放电中观察到了NO (A—X)的谱线,但在N2+02及空气放电中该谱线强度要弱很多,而且在O2气放电中未测到NO (A—X),因为氧气含量较高时NO与02、O3或O原子继续反应生成NO2而被减少,且随氧气含量的增加而迅速减少。
(3)对甲基紫脱色处理结果表明,甲基紫溶液脱色率由高到低依次为O2>He+O2>He,且He+O2混合气和单纯02气放电下的脱色率相差不大。He气放电消耗的能量密度低,但脱色率小于50%；O2气放电处理甲基紫溶液脱色率达99.5%,但是消耗的能量密度高达32.5kJ/L; He+O2混合气放电处理甲基紫溶液体现了很好的脱色效果同时能量消耗较低,处理180s时脱色率达96%而能量消耗却只有7.7kJ／L。因此提出He+02混合气为最佳用于甲基紫溶液脱色的放电气体组合,既能取得高脱色率又能降低能耗。
对甲基紫的降解机理分析得出,OH基和02对甲基紫的降解起着关键作用,而OH基主要通过与氧有关的反应获得,因此与活性氧的含量有关。因此认为活性氧(如O2-·、H2O2、OH、O等)是甲基紫脱色的关键粒子。
(4)利用自制的DBD装置结合选择催化还原(SCR)装置建立了多功能的DBD协同SCR脱除NOx研究平台。分别以C2H5OH和C3H6为还原剂、以Ag/Al2O3为催化剂,研究了高NOx浓度(800ppm左右)及高空速(50000h-1)下,DBD等离子体协同SCR脱除NOx的特性及反应机理,同时考察了尾气温度对NOx脱除的影响,并重点研究了150℃低温时的NOx脱除特性,及利用]FTIR光谱分析了反应产物。
DBD等离子体协同SCR作用在低温时取得了很好的脱除效果。C2H5OH为还原剂,在含8%H2O且温度150℃的模拟柴油机尾气中NOx脱除率高达80%,其中NO脱除率高达90%。C3H6为还原剂,尾气中不含水时NOx脱除率最高达88%,NO脱除率高达94%,但加入8%H2O后NOx脱除率降低至60%。对FTIR吸收光谱的分析进一步确认了SCR单独作用在低温时对NOx脱除无效,而DBD协同SCR却能有效脱除NOx,同时也脱除了碳氢,NOx及碳氢脱除后的最终产物主要为N2、C02和H2O。
通过对比研究DBD和SCR分别作用及协同作用时的NOx脱除特性,提出NOx脱除机理为：放电形成时等离子体中的强氧化性粒子与碳氢作用生成的有机活性基团(主要为CH3O2)在催化剂促进下迅速将NO氧化成NO2；随着电压升高,NO2在催化剂表面与碳氢作用生成活性中间产物CxHyNzO,NO2含量越高则生成的活性中间产物越多；放电在活化气体的同时也提高了催化床的温度,从而间接提高了催化剂的活性,最终NOx在催化剂促进下被CxHyNzO脱除,同时CxHyNzO被转化为CO2和H2O而脱除。实验证明了低温时等离子体中强氧化性粒子O3、HO2等对NO的作用很弱,而被DBD活化的碳氢才是NO有效氧化的关键粒子。
With the rapid development of economy and society in the world, the environmental pollution is increasingly serious and harmful to the human living environment and health, so various countries are formulating increasingly strict emission rule. Now, in our country it is commonly difficult for the decoloration of waste water and for the removal of NOx in diesel engine exhaust gases.
Dielectric Barrier Discharges (DBD) plasma which includes energetic electrons and active particles is effective and environmental techniques of handling. In this paper, the author developed DBD device and matched power supply source, whereby the characteristics and emission spectrums of various gases discharge were studied, and the related investigations were taken for the decoloration of waste water and the removal of NOx in diesel engine exhaust gases. In general, the achieved achievements were mainly as follows:
(1) The DBD device and its matched power supply source was developed, and by the device the research platform of DBD was build.
(2) The characteristics and emission spectrums of discharge in Ar, Ar+O2, He, He+02, N2, N2+O2, O2, and air were studied. Results show discharge is similar glow in He gas and filar in the others. The intense spectral line of N atom whose lifetime is short was observed in Ar and Ar+O2 discharge, and the reactive OH radical was observed in Ar discharge but not in the others, so it might be more value in application. Additionally, the spectral line of NO(A—X) was observed in N2, N2+O2, and air discharge, and the intensity of spectral line rapidly decreased with the increasing scale of O2 gas.
(3) The results of decoloration for methyl violet show that the decoloration ratio from high to low was O2, He+02 and He, and the effect was similar in He+O2 and O2 gas discharge. For He gas discharge, consumed energy density is low, but the decoloration ratio is also lower than 50%; for O2 gas discharge, the decoloration ratio of 99.5% was achieved, but the high energy density of 32.5kJ/L was required; for He+02 discharge, the decoloration ratio of 96% was achieved, but the consumed energy density was only 7.7kJ/L. So we propose that the mixed gases of He+02 are optimal for the decoloration of methyl violet, because the high decoloration ratio can be achieved and low energy density will be cost in the system.
By analyzing the decoloration mechanism of methyl violet, it is considered that OH radical and O2 gas play a key role in the decoloration, and OH radical is mainly got by the reactions related with O. So we consider the reactive oxygen (such as O2-·,H2O2, OH, O) as the key particles for the decoloration of methyl violet.
(4) Using the self-developed DBD device combined with selective catalytic reduction (SCR) device, we build a research platform of DBD cooperating with SCR for NOx removal. The characteristics of NOx removal and reaction mechanisms by DBD cooperated with SCR were investigated under the conditions of high NOx concentration (800 ppm) and high space velocity (50000 h-1). Meanwhile, the effect of temperature on NOx removal was also studied, especially the NOx removal at the low temperature of 150℃was investigated and the reaction products were analyzed by FTIR spectra.
By DBD cooperated with SCR the high NOx removal rate was achieved at low temperature. With C2H5OH as reductant, the NOx removal rate of 80% and the NO removal rate of 90% were achieved at 150℃when 8% H2O was fed into the exhaust gases. With C3H6 as reductant, the NOx removal rate of 88% and the NO removal rate of 94% were achieved at 150℃in dry gases, but the NOx removal rate decreased to 60% when 8% H2O was fed into the exhaust gases. The FTIR spectra confirm the NOx can effectively be removed by DBD cooperated with SCR, and the reaction products are mainly N2, CO2 and H2O.
By contrast research on DBD and SCR individually and together impacting on NOx removal, the reaction mechanism of NOx removal were proposed as follows:when discharge came into being, strong oxidative particles in plasma reacted with hydrocarbons to get organic reactive particles which rapidly oxidized NO to NO2 at the acceleration of catalyst; NO2 reacted with hydrocarbons to get CxHyNzO compound over catalysts, and the more NO2 the more CxHyNzO compound were produced; discharge resulted in the activation of hydrocarbons and the rise of catalyst bed temperature, so finally the NOx was removed by reaction with CxHyNzO over catalyst, and simultaneously the hydrocarbons were removed by the generation of CO2 and H2O.Experiments show the role of O3, HO2, and so on in plasma is weak in reaction with NO, and the hydrocarbons are just the key particles for the effective oxidation of NO to NO2.
引文
参考文献
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