LED-紫外线/氯高级氧化降解苯妥英钠特性
|
摘要
发光二极管(light emitting diode,LED)作为新型紫外线光源,其与活性氯联用的LED-紫外线/氯高级氧化技术可协同高效降解抗惊厥药微量污染物苯妥英钠(phenytoin sodium,PHT)。LED-紫外线剂量为0. 82 J/cm~2时,LED-紫外线/氯高级氧化对水中的PHT去除率到62%,远高于单独氯化和单独LED-紫外线处理的加和。降解动力学研究发现:LED-紫外线/氯高级氧化降解PHT符合准一级反应动力学。280 nm LED作为光源的LED-紫外线/氯相比310 nm LED-紫外线/氯有更好的PHT去除效果。与LED-紫外线/H_2O_2和LED-紫外线/过硫酸盐相比,氧化剂(氯、H_2O_2和过硫酸盐)浓度为0. 282 mmol/L时,LED-紫外线/氯高级氧化降解PHT的准一级反应动力学常数(0. 096 min~(-1))远高于LED-紫外线/H_2O_2和LED-紫外线/过硫酸盐,分别是其3. 7倍和3. 0倍。优化氯投加量发现,LED-紫外线/氯高级氧化在较低氯投加量(10 mg/L)条件下即可高效降解PHT。对PHT毒性变化研究发现,氯化作用降解PHT过程中,可生成具有急性毒性的中间产物,且持续累积。LED-紫外线/氯高级氧化降解PHT在较低紫外线剂量(0. 08 J/cm~2)下生成了具有急性毒性的中间产物,随着紫外线剂量增加至0. 41 J/cm~2,毒性中间产物被有效去除。
LED-UV/chlorine advanced oxidation process combining light emitting diode( LED),as a new type of ultraviolet light source with active chlorine,was found to be able to efficiently degradate anticonvulsant drug micro pollutant phenytoin sodium( PHT). LED-UV/chlorine advanced oxidation process could remove 62% of PHT under the LED-UV dosage of 0. 82 J/cm~2,which was far higher than the sum of single chlorination and single LED-UV radiation. It's discovered in the study of degradation kinetics that the degradation of PHT by LED-UV/chlorine advanced oxidation process conformed to pseudo-first-order reaction kinetics. 280 nm LED-UV/chlorine had a better PHT removal effect than 310 nm LED-UV/chlorine. Compared to LED-UV/H_2O_2 and LED-UV/persulfate,with same oxidant dosage of 0. 282 mmol/L,the pseudo-firstorder reaction kinetics constant( 0. 096 min~(-1)) of LED-UV/chlorine advanced oxydative degradation of PHT was 3. 7 and 3. 0 times higher than that of LED-UV/H_2O_2 and LED-UV/persulfate respectively. It's discovered from the optimization of chlorine dosage that,LED-UV/chlorine advanced oxidation could significantly degradate PHT with a lower chlorine dosage of 10 mg/L.It's discovered in the study on toxicity change of PHT that,in the degradation of PHT with chlorination,intermediate products with acute toxicity were generated and continued to accumulate. In the degradation of PHT by LED-UV/chlorine,the intermediate products with acute toxicity were generated under a lower ultraviolet dosage of 0. 08 J/cm~2,and with the increase of ultraviolet dosage to 0. 41 J/cm~2,toxic intermediate products could be efficiently removed.
LED-UV/chlorine advanced oxidation process combining light emitting diode( LED),as a new type of ultraviolet light source with active chlorine,was found to be able to efficiently degradate anticonvulsant drug micro pollutant phenytoin sodium( PHT). LED-UV/chlorine advanced oxidation process could remove 62% of PHT under the LED-UV dosage of 0. 82 J/cm~2,which was far higher than the sum of single chlorination and single LED-UV radiation. It's discovered in the study of degradation kinetics that the degradation of PHT by LED-UV/chlorine advanced oxidation process conformed to pseudo-first-order reaction kinetics. 280 nm LED-UV/chlorine had a better PHT removal effect than 310 nm LED-UV/chlorine. Compared to LED-UV/H_2O_2 and LED-UV/persulfate,with same oxidant dosage of 0. 282 mmol/L,the pseudo-firstorder reaction kinetics constant( 0. 096 min~(-1)) of LED-UV/chlorine advanced oxydative degradation of PHT was 3. 7 and 3. 0 times higher than that of LED-UV/H_2O_2 and LED-UV/persulfate respectively. It's discovered from the optimization of chlorine dosage that,LED-UV/chlorine advanced oxidation could significantly degradate PHT with a lower chlorine dosage of 10 mg/L.It's discovered in the study on toxicity change of PHT that,in the degradation of PHT with chlorination,intermediate products with acute toxicity were generated and continued to accumulate. In the degradation of PHT by LED-UV/chlorine,the intermediate products with acute toxicity were generated under a lower ultraviolet dosage of 0. 08 J/cm~2,and with the increase of ultraviolet dosage to 0. 41 J/cm~2,toxic intermediate products could be efficiently removed.
引文
[1] Deo R P,Halden R U. Pharmaceuticals in the built and natural water environment of the United States[J]. Water,2013,5(3):1346-1365.
[2] Murray K E,Thomas S M,Bodour A A. Prioritizing research for trace pollutants and emerging contaminants in the freshwater environment[J]. Environmental Pollution,2010,158(12):3462-3471.
[3] Yuan S,Jiang X,Xia X,et al. Detection,occurrence and fate of22 psychiatric pharmaceuticals in psychiatric hospital and municipal wastewater treatment plants in Beijing, China[J].Chemosphere,2013,90(10):2520-2525.
[4] Brodin T,Fick J,Jonsson M,et al. Dilute concentrations of a psychiatric drug alter behavior of fish from natural populations[J].Science,2013,339(6121):814-815.
[5] Klavarioti M,Mantzavinos D,Kassinos D. Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes[J]. Environment International,2009,35(2):402-417.
[6] Fang J, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/Free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[7] Shu Z,Li C,Belosevic M,et al. Application of a solar UV/Chlorine advanced oxidation process to oil sands process-affected water remediation[J]. Environmental Science&Technology,2014,48(16):9692-9701.
[8] Jin J,El-Din M G,Bolton J R. Assessment of the UV/Chlorine process as an advanced oxidation process[J]. Water Research,2011,45(4):1890-1896.
[9] Fang J, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/Free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[10] Chan P Y,Gamal El-Din M,Bolton J R. A solar-driven UV/Chlorine advanced oxidation process[J]. Water Research,2012,46(17):5672-5682.
[11] Wang W L,Wu Q Y,Li Z M,et al. Light-emitting diodes as an emerging UV source for UV/chlorine oxidation:carbamazepine degradation and toxicity changes[J]. Chemical Engineering Journal,2016,310:148-156.
[12]国家环境保护局.GB/T 15441—1995:水质急性毒性的测定发光细菌法[S].北京:中国标准出版社,1995.
[13] Bolton J R,Stefan M I,Shaw P,et al. Determination of the quantum yields of the potassium ferrioxalate and potassium iodideiodate actinometers and a method for the calibration of radiometer detectors[J]. Journal of Photochemistry and Photobiology A:Chemistry,2011,222(1):166-169.
[14]王婷,吴乾元,王文龙,等.紫外线/氯高级氧化降解甲基异噻唑啉酮[J].环境工程学报,2017,11(1):21-26.
[15] Munch D J,Hautman D P. Method 551. 1. Determination of chlorination disinfection byproducts, chlorinated solvents, and halogenated pesticides/herbicides in drinking water by liquid-liquid extraction and gas chromatography with electron-capture detection(Revision 1. 0)[S]. Washington,DC:Office of Research and Development,US Environmental Protection Agency,1995.
[16] Goldstein S,Aschengrau D,Diamant Y,et al. Photolysis of aqueous H2O2:quantum yield and applications for polychromatic UV actinometry in photoreactors[J]. Environmental Science&Technology,2007,41(21):7486-7490.
[17] Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science&Technology,2004,38(13):3705-3712.
[18] Kong X,Jiang J,Ma J,et al. Degradation of atrazine by UV/chlorine:efficiency,influencing factors,and products[J]. Water Research,2016,90:15-23.
[19] Fang J Y,Fu Y,Shang C. The roles of reactive species in micropollutant degradation in the UV/free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[20] Deng L,Huang C H,Wang Y L. Effects of combined UV and chlorine treatment on the formation of trichloronitromethane from amine precursors[J]. Environmental Science&Technology,2014,48(5):2697-2705.
[2] Murray K E,Thomas S M,Bodour A A. Prioritizing research for trace pollutants and emerging contaminants in the freshwater environment[J]. Environmental Pollution,2010,158(12):3462-3471.
[3] Yuan S,Jiang X,Xia X,et al. Detection,occurrence and fate of22 psychiatric pharmaceuticals in psychiatric hospital and municipal wastewater treatment plants in Beijing, China[J].Chemosphere,2013,90(10):2520-2525.
[4] Brodin T,Fick J,Jonsson M,et al. Dilute concentrations of a psychiatric drug alter behavior of fish from natural populations[J].Science,2013,339(6121):814-815.
[5] Klavarioti M,Mantzavinos D,Kassinos D. Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes[J]. Environment International,2009,35(2):402-417.
[6] Fang J, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/Free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[7] Shu Z,Li C,Belosevic M,et al. Application of a solar UV/Chlorine advanced oxidation process to oil sands process-affected water remediation[J]. Environmental Science&Technology,2014,48(16):9692-9701.
[8] Jin J,El-Din M G,Bolton J R. Assessment of the UV/Chlorine process as an advanced oxidation process[J]. Water Research,2011,45(4):1890-1896.
[9] Fang J, Fu Y, Shang C. The roles of reactive species in micropollutant degradation in the UV/Free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[10] Chan P Y,Gamal El-Din M,Bolton J R. A solar-driven UV/Chlorine advanced oxidation process[J]. Water Research,2012,46(17):5672-5682.
[11] Wang W L,Wu Q Y,Li Z M,et al. Light-emitting diodes as an emerging UV source for UV/chlorine oxidation:carbamazepine degradation and toxicity changes[J]. Chemical Engineering Journal,2016,310:148-156.
[12]国家环境保护局.GB/T 15441—1995:水质急性毒性的测定发光细菌法[S].北京:中国标准出版社,1995.
[13] Bolton J R,Stefan M I,Shaw P,et al. Determination of the quantum yields of the potassium ferrioxalate and potassium iodideiodate actinometers and a method for the calibration of radiometer detectors[J]. Journal of Photochemistry and Photobiology A:Chemistry,2011,222(1):166-169.
[14]王婷,吴乾元,王文龙,等.紫外线/氯高级氧化降解甲基异噻唑啉酮[J].环境工程学报,2017,11(1):21-26.
[15] Munch D J,Hautman D P. Method 551. 1. Determination of chlorination disinfection byproducts, chlorinated solvents, and halogenated pesticides/herbicides in drinking water by liquid-liquid extraction and gas chromatography with electron-capture detection(Revision 1. 0)[S]. Washington,DC:Office of Research and Development,US Environmental Protection Agency,1995.
[16] Goldstein S,Aschengrau D,Diamant Y,et al. Photolysis of aqueous H2O2:quantum yield and applications for polychromatic UV actinometry in photoreactors[J]. Environmental Science&Technology,2007,41(21):7486-7490.
[17] Anipsitakis G P, Dionysiou D D. Radical generation by the interaction of transition metals with common oxidants[J].Environmental Science&Technology,2004,38(13):3705-3712.
[18] Kong X,Jiang J,Ma J,et al. Degradation of atrazine by UV/chlorine:efficiency,influencing factors,and products[J]. Water Research,2016,90:15-23.
[19] Fang J Y,Fu Y,Shang C. The roles of reactive species in micropollutant degradation in the UV/free chlorine system[J].Environmental Science&Technology,2014,48(3):1859-1868.
[20] Deng L,Huang C H,Wang Y L. Effects of combined UV and chlorine treatment on the formation of trichloronitromethane from amine precursors[J]. Environmental Science&Technology,2014,48(5):2697-2705.
© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号 地址：北京市海淀区学院路29号 邮编：100083 电话：办公室：(+86 10)66554848；文献借阅、咨询服务、科技查新：66554700 |