高压脉冲电晕降解液相苯酚的试验研究
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摘要
高压脉冲电晕放电等离子体处理有机废水技术是一种新型的高级氧化技术,除了放电产生的活性粒子能够作用于有机污染物之外,它还兼具紫外光解,臭氧,等效应,近年来已成为等离子体技术研究的热点。苯酚是我国规定的水中优先控制的污染物,本文选定苯酚作为目标污染物,通过对比其它的含酚废水处理技术,指出了高压脉冲电晕放电等离子体技术的优势。
本文从电源与反应器的匹配性、电源特性、反应器特性以及溶液特性等几个方面对高压脉冲放电等离子体降解苯酚进行了系统的实验研究;通过对降解中间产物的分析,对其降解途径进行了探讨。
本文采用三维电极进行放电试验时,可以形成稳定的电晕流光,电晕在反应器空间内的充盈度好,电晕区间大,所处理的废水量大而且可以处于流动状态,电源与反应器的匹配性很好。
在高压脉冲放电的前提下,向溶液中添加Fe~(2+)、Fe~(3+)以及H_2O_2均可以提高苯酚的降解效率。本试验中添加Fe~(2+)后,由于形成芬顿(Fenton)效应,苯酚降解效率提高幅度最大,其次为Fe~(3+),H_2O_2对苯酚降解效率的提高幅度最小。苯酚降解效率随着Fe~(2+)添加量的增加呈现先上升后下降的趋势。Fe~(2+)浓度为0.015×10~(-3)mol/L,采用三维电极,电极外径Φ0.7mm,脉冲峰值电压为40kV,脉冲频率180Hz,放电间距25mm,曝气为氧气,速率6L/min,溶液初始电导率为6μs/cm,pH值是6,经过处理120min后的苯酚降解效率可以达到94.39%。
提高脉冲电压峰值或者提高脉冲频率均可以提高苯酚的降解效率,通过对脉冲电容有效能量的研究显示,提高脉冲电压对苯酚的降解效率影响更大。增加电极个数,增加曝气速率,减小溶液电导率及适当减小电极外径,均有利于提高苯酚的降解效率。
在高压脉冲电晕等离子体对苯酚的降解过程中,首先是羟基自由基攻击苯酚分子,生成对苯二酚或者邻苯二酚,对苯二酚和邻二苯酚进一步被氧化生成苯二甲酸二乙酯。其后苯二甲酸二乙酯继续被氧化,苯环开环,开环产物可以被进一步氧化生成亚甲基乙酸、丙酮等物质,并最终被氧化分解为CO_2和H_2O。
The pulsed high-voltage corona discharge is a new technology of advanced oxidation technology in the field of organic waste-water treatment.The corona discharge can produce·OH, UV,ozone and other effects of oxidation to degradate the organic pollutants.Plasma technology has become a hot research field in recent years.This paper selected phenol as the target pollutant in water,introduced the hazards of phenol-containing water,pointed out the advantages of high-voltage pulsed corona discharge technology by comparing other waste-water treatment technologies.
Some aspects of the high-voltage pulsed corona discharge to remove phenol were studied in this paper,such as power reactor,the matching between the power and the reactor,and the solution features.The degradation way of the phenol were discussed through analyzed the intermediate.Main conclusions are as follows:
Corona discharged stably,the corona was wide,and could fill the space of reactor well when using three-dimensional electrode.The treated waste water was in the state of flowing. The match between power and reactor was good.
Added Fe~(2+),Fe~(3+) and H_2O_2 could improve the efficiency of the degradation of phenol when use high-voltage pulsed corona discharge to treat waste-water.When added Fe~(2+),the raising extent of phenol degradation was the best,due to the formation of Fenton effect,followed by Fe~(3+),and H_2O_2 was the smallest.With the increase of the addition of the Fe~(2+),the efficiency of phenol degradation rose first,and then it went down.When used a three-dimensional electrode, electrode diameter wasΦ0.7 mm,pulsed peak voltage was 42 kV,pulsed frequency was 180 Hz, discharge spacing was 25 mm,oxygen as the bubbling gas,the rate was 6 L/min,Fe~(2+) concentration was 0.015×10~(-3)mol/L,the initial solution conductivity was 6μs/cm,pH value was 6,the efficiency of phenol degradation could reach 94.39%after 120 min treatment.
The efficiency of the phenol degradation improved when increased the peak of pulsed voltage or pulsed frequency.Compared to the pulsed frequency,the pulsed voltage played a more important role to the degradation efficiency.Increase the number of electrodes,the rate of the bubbling gas,reduce the electrical conductivity and reduce electrode diameter appropriately, are all conducive to improving the efficiency of the phenol degradation.
When use high-voltage pulsed corona plasma to degradate the phenol,first,the hydroxyl radical attacks the phenol molecules,form hydroquinone or adjacent phenol.Hydroquinone or adjacent phenol can be further oxidative and form diethyl phthalate.Diethyl phthalate then continue to be oxidated,benzene ring open and induce open-ring products,and then they can be further oxidated,generate Asia-acetic acid,acetone and other substances,eventually broken down into CO_2 and H_2O.
本文从电源与反应器的匹配性、电源特性、反应器特性以及溶液特性等几个方面对高压脉冲放电等离子体降解苯酚进行了系统的实验研究;通过对降解中间产物的分析,对其降解途径进行了探讨。
本文采用三维电极进行放电试验时,可以形成稳定的电晕流光,电晕在反应器空间内的充盈度好,电晕区间大,所处理的废水量大而且可以处于流动状态,电源与反应器的匹配性很好。
在高压脉冲放电的前提下,向溶液中添加Fe~(2+)、Fe~(3+)以及H_2O_2均可以提高苯酚的降解效率。本试验中添加Fe~(2+)后,由于形成芬顿(Fenton)效应,苯酚降解效率提高幅度最大,其次为Fe~(3+),H_2O_2对苯酚降解效率的提高幅度最小。苯酚降解效率随着Fe~(2+)添加量的增加呈现先上升后下降的趋势。Fe~(2+)浓度为0.015×10~(-3)mol/L,采用三维电极,电极外径Φ0.7mm,脉冲峰值电压为40kV,脉冲频率180Hz,放电间距25mm,曝气为氧气,速率6L/min,溶液初始电导率为6μs/cm,pH值是6,经过处理120min后的苯酚降解效率可以达到94.39%。
提高脉冲电压峰值或者提高脉冲频率均可以提高苯酚的降解效率,通过对脉冲电容有效能量的研究显示,提高脉冲电压对苯酚的降解效率影响更大。增加电极个数,增加曝气速率,减小溶液电导率及适当减小电极外径,均有利于提高苯酚的降解效率。
在高压脉冲电晕等离子体对苯酚的降解过程中,首先是羟基自由基攻击苯酚分子,生成对苯二酚或者邻苯二酚,对苯二酚和邻二苯酚进一步被氧化生成苯二甲酸二乙酯。其后苯二甲酸二乙酯继续被氧化,苯环开环,开环产物可以被进一步氧化生成亚甲基乙酸、丙酮等物质,并最终被氧化分解为CO_2和H_2O。
The pulsed high-voltage corona discharge is a new technology of advanced oxidation technology in the field of organic waste-water treatment.The corona discharge can produce·OH, UV,ozone and other effects of oxidation to degradate the organic pollutants.Plasma technology has become a hot research field in recent years.This paper selected phenol as the target pollutant in water,introduced the hazards of phenol-containing water,pointed out the advantages of high-voltage pulsed corona discharge technology by comparing other waste-water treatment technologies.
Some aspects of the high-voltage pulsed corona discharge to remove phenol were studied in this paper,such as power reactor,the matching between the power and the reactor,and the solution features.The degradation way of the phenol were discussed through analyzed the intermediate.Main conclusions are as follows:
Corona discharged stably,the corona was wide,and could fill the space of reactor well when using three-dimensional electrode.The treated waste water was in the state of flowing. The match between power and reactor was good.
Added Fe~(2+),Fe~(3+) and H_2O_2 could improve the efficiency of the degradation of phenol when use high-voltage pulsed corona discharge to treat waste-water.When added Fe~(2+),the raising extent of phenol degradation was the best,due to the formation of Fenton effect,followed by Fe~(3+),and H_2O_2 was the smallest.With the increase of the addition of the Fe~(2+),the efficiency of phenol degradation rose first,and then it went down.When used a three-dimensional electrode, electrode diameter wasΦ0.7 mm,pulsed peak voltage was 42 kV,pulsed frequency was 180 Hz, discharge spacing was 25 mm,oxygen as the bubbling gas,the rate was 6 L/min,Fe~(2+) concentration was 0.015×10~(-3)mol/L,the initial solution conductivity was 6μs/cm,pH value was 6,the efficiency of phenol degradation could reach 94.39%after 120 min treatment.
The efficiency of the phenol degradation improved when increased the peak of pulsed voltage or pulsed frequency.Compared to the pulsed frequency,the pulsed voltage played a more important role to the degradation efficiency.Increase the number of electrodes,the rate of the bubbling gas,reduce the electrical conductivity and reduce electrode diameter appropriately, are all conducive to improving the efficiency of the phenol degradation.
When use high-voltage pulsed corona plasma to degradate the phenol,first,the hydroxyl radical attacks the phenol molecules,form hydroquinone or adjacent phenol.Hydroquinone or adjacent phenol can be further oxidative and form diethyl phthalate.Diethyl phthalate then continue to be oxidated,benzene ring open and induce open-ring products,and then they can be further oxidated,generate Asia-acetic acid,acetone and other substances,eventually broken down into CO_2 and H_2O.
引文
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