介质阻挡放电优化激活过硫酸盐处理四环素废水
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摘要
为了优化介质阻挡放电激活过硫酸盐处理四环素废水,选择放电电压、溶液初始pH值和过硫酸盐投加量为自变量,以四环素的去除率为响应值,采用响应曲面法Box-Behnken设计原理对介质阻挡放电激活过硫酸盐降解四环素的效果进行分析。结果表明影响四环素去除率大小因素的顺序为放电电压>过硫酸盐投加量>溶液初始pH值。根据模型确定了废水中四环素的降解优化条件如下:放电电压18.0 kV,溶液初始pH 8.48,过硫酸盐投加量138.89mg,四环素去除率达95.9%。四环素的氧化降解过程符合一级反应动力学。溶液初始pH值为3.9、5.9时,降解四环素的主要自由基为SO_4~–·;溶液初始pH值为7.3、8.3时,降解四环素的主要自由基为SO_4~–·与·OH;当溶液初始pH为10.5时,降解四环素的主要自由基为·OH。
In order to realize the optimized activation of persulfate by dielectric barrier discharge(DBD) for the treatment of tetracycline wastewater, the discharge voltage, the initial pH value of the solution and the persulfate dosage were selected as the independent variables, and the removal of tetracycline was as the response value. The effect of tetracycline degradation with persulfate activated by DBD was analyzed using the response surface method Box-Behnken design principle. The experimental results show that the order of the factors affecting the removal rate of tetracycline is as follows:the discharge voltage>persulfate dosage>initial pH value of the solution. The optimal conditions for the degradation of tetracycline in wastewater are as follows: discharge voltage 18.0 kV, initial solution pH 8.48, persulfate dosage 138.89 mg, and the tetracycline removal rate reaches 95.9% under optimized conditions. The oxidative degradation of tetracycline accords with the first-order reaction kinetics. When the initial solution p H=3.9 and 5.9, the main free radical for degrading tetracycline is SO_4~–·, when the initial solution pH=7.3 and 8.3, the main free radicals for degrading tetracycline are SO_4~–· and ·OH; when the initial solution pH is 10.5, the main free radical for degrading tetracycline is ·OH.
In order to realize the optimized activation of persulfate by dielectric barrier discharge(DBD) for the treatment of tetracycline wastewater, the discharge voltage, the initial pH value of the solution and the persulfate dosage were selected as the independent variables, and the removal of tetracycline was as the response value. The effect of tetracycline degradation with persulfate activated by DBD was analyzed using the response surface method Box-Behnken design principle. The experimental results show that the order of the factors affecting the removal rate of tetracycline is as follows:the discharge voltage>persulfate dosage>initial pH value of the solution. The optimal conditions for the degradation of tetracycline in wastewater are as follows: discharge voltage 18.0 kV, initial solution pH 8.48, persulfate dosage 138.89 mg, and the tetracycline removal rate reaches 95.9% under optimized conditions. The oxidative degradation of tetracycline accords with the first-order reaction kinetics. When the initial solution p H=3.9 and 5.9, the main free radical for degrading tetracycline is SO_4~–·, when the initial solution pH=7.3 and 8.3, the main free radicals for degrading tetracycline are SO_4~–· and ·OH; when the initial solution pH is 10.5, the main free radical for degrading tetracycline is ·OH.
引文
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[5]WANG X,JIA J,WANG Y.Combination of photo catalysis with hydrodynamic cavitation for degradation of tetracycline[J].Chemical Engineering Journal,2017,315:274-282.
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[13]孙明,郝夏桐,鲁晓辉,等.气液两相脉冲放电反应器的设计及其对酸性橙Ⅱ的降解效果[J].高电压技术,2015,41(2):498-503.SU Ming,HAO Xiatong,LU Xiaohui,et al.A reactor design of gas-liquid two-phase pulse discharge and its performance in degrading Acid OrangeⅡ[J].High Voltage Engineering,2015,41(2):498-503.
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[15]汪超,王铁成,屈广周,等.脉冲电晕放电等离子体耦合土壤颗粒去除废水中盐酸四环素[J].高电压技术,2018,44(9):3076-3082.WANG Chao,WANG Tiecheng,QU Guangzhou,et al.Removal of tetracycline HCl in wastewater by pulsed corona discharge plasma coupled with soil particles[J].High Voltage Engineering,2018,44(9):3076-3082.
[16]CHEN J,DU Y,SHEN Z,et al.Non-thermal plasma and Bi PO4 induced degradation of aqueous crystal violet[J].Separation and Purification Technology,2017,179:135-144.
[17]杨长河,刘健辉,曹志荣,等.DBD高级氧化耦合活性炭吸附处理水中碱性品红[J].高电压技术,2016,42(2):392-397.YANG Changhe,LIU Jianhui,CAO Zhirong,et al.Treatment of fuchsin basic in water by DBD advanced oxidation coupling with activated carbon adsorption[J].High Voltage Engineering,2016,42(2):392-397.
[18]VANRAES P,GHODBANE H,DAVISTER D,et al.Removal of several pesticides in a falling water film DBD reactor with activated carbon textile:Energy efficiency[J].Water Research,2017,116:1-12.
[19]董冰岩,邓苇,孙宇史,等.高压脉冲放电协同纳米催化剂降解苯酚废水[J].高电压技术,2017,43(8):2645-2652.DONG Bingyan,DENG Wei,SUN Yushi,et al.Phenol wastewater treatment by high voltage pulse discharge combined with nanometer catalyst[J].High Voltage Engineering,2017,43(8):2645-2652.
[20]施宸菲,薛瑞杰,李雨濛,等.不同活性炭活化过硫酸盐的效能及机理的规律研究[J].环境科学学报,2018,38(4):1501-1508.SHI Chenfei,XUE Ruijie,LI Yumeng,et al.Study on the efficiency and mechanism of persulfate activation by different activated carbon[J].Acta Scientiae Circumstantiae,2018,38(4):1501-1508.
[21]LIU Y,HE X,FU Y,et al.Kinetics and mechanism investigation on the destruction of oxytetracycline by UV-254nm activation of persulfate[J].Journal of Hazardous Materials,2016,305:229-239.
[22]NIE M,YANG Y,ZHANG Z,et al.Degradation of chloramphenicol by thermally activated persulfate in aqueous solution[J].Chemical Engineering Journal,2014,246:373-382.
[23]EPOLD I,TRAPIDO M,DULOVA N.Degradation of levofloxacin in aqueous solutions by Fenton,ferrous ion-activated persulfate and combined Fenton/persulfate systems[J].Chemical Engineering Journal,2015,279:452-462.
[24]SHANG K,WANG X,LI J,et al.Synergetic degradation of Acid Orange 7(AO7)dye by DBD plasma and persulfate[J].Chemical Engineering Journal,2017,311:378-384.
[25]SHANG K,WANG H,LI J,et al.Activation of peroxydisulfate by gas-liquid pulsed discharge plasma to enhance the degradation of p-nitrophenol[J].Plasma Science and Technology,2017,19(6):064017.
[26]SON G,LEE H.Methylene blue removal by submerged plasma irradiation system in the presence of persulfate[J].Environmental Science and Pollution Research,2016,23(15):15651-15656.
[27]TANG S,YUAN D,RAO Y,et al.Persulfate activation in gas phase surface discharge plasma for synergetic removal of antibiotic in water[J].Chemical Engineering Journal,2018,337:446-454.
[28]张占梅.基于超声辐射的高级氧化技术处理偶氮染料酸性绿B的试验研究[D].重庆:重庆大学,2009.ZHANG Zhanmei.Experimental study on treatment of azo dye Acid Green B by advanced oxidation processes based on ultrasonic irradiation[D].Chongqing,China:Chongqing University,2009.
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