Cu<sup>2+</sup>强化UV活化过氧乙酸降解水中的双氯芬酸

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Abstract The degradation of diclofenac (DCF) by Cu²⁺ enhanced UV activation of peracetic acid (Cu²⁺/UV/PAA) was investigated. The effects of pH, PAA dose, Cu²⁺ dose, inorganic anions (such as Cl^-, SO₄^2-, NO₃^- and CO₃^2-) and dissolved organic matter (DOM) on DCF removal by Cu²⁺/UV/PAA were also evaluated. The degradation products and transformation mechanism of DCF by Cu²⁺/UV/PAA were studied. Both UV and Cu²⁺ could activate PAA to produce active radicals, which could promote DCF removal. The degradation of DCF by Cu²⁺/UV/PAA followed the pseudo first-order kinetics and its degradation was probably attributed to direct photolysis, HO^· oxidation and other radicals oxidation such as CH₃COO^· and CH₃COOO^·. In the pH range of 3-11, DCF had the best degradation efficiency at pH 8.5. When PAA dose increased, the degradation efficiency of DCF was enhanced gradually, but excessive PAA could compete with DCF for HO^·. The increase of Cu²⁺ dose could also promote DCF removal, while excessive Cu²⁺ could form Cu(OH)₂, which might lead to the reduction of its catalytic ability. Since NO₃^- can generate HO^· under UV irradiation, its existence promoted the degradation of DCF, and the enhancement effect increased with the increase in its concentration. The presence of Cl^-, SO₄^2-, CO₃^2- and DOM in different concentrations had little effect on DCF removal. Thirteen degradation products were detected in the degradation of DCF by Cu²⁺/UV/PAA. According to these degradation products, the probable transformation mechanism of DCF was proposed exhibiting eight reaction pathways.

Key words： diclofenac UV peracetic acid Cu²⁺ hydroxyl radical transformation mechanism

Received: 10 April 2020

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X703

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	ZHANG Li
	FU Yong-sheng
	LIU Yi-qing

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ZHANG Li,FU Yong-sheng,LIU Yi-qing. Degradation of diclofenac in water by Cu²⁺ enhanced UV activation of peracetic acid[J]. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(12): 5260-5269.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2020/V40/I12/5260

[1]	夏文君,徐劼,刘锋,等.秸秆生物碳对双氯芬酸钠的吸附性能研究[J]. 中国环境科学, 2019,39(3):1054-1060. Xia W J, Xu J, Liu F, et al. Adsorption of diclofenac on straw-biochar[J]. China Environmental Science, 2019,39(3):1054-1060.
[2]	Hua Z, Dai Z, Bai X, et al. Copper nanoparticles sensitized TiO2 nanotube arrays electrode with enhanced photoelectrocatalytic activity for diclofenac degradation[J]. Chemical Engineering Journal, 2016, 283:514-523.
[3]	Zhang Y, Geisen S U, Gal C. Carbamazepine and diclofenac:Removal in wastewater treatment plants and occurrence in water bodies[J]. Chemosphere, 2008,73(8):1151-1161.
[4]	Schwaiger J, Ferling H, Mallow U, et al. Toxic effects of the non-steroidal anti-inflammatory drug diclofenac:Part Ⅰ:histopathological alterations and bioaccumulation in rainbow trout[J]. Aquatic Toxicology, 2004,68(2):141-150.
[5]	Ericson H, Thorsen G, Kumblad L, et al. Physiological effects of diclofenac, ibuprofen and propranolol on Baltic Sea blue mussels[J]. Aquatic Toxicology, 2010,99(2):223-231.
[6]	Cardoso-Vera J D, Islas-Flores H, SanJuan-Reyes N, et al. Comparative study of diclofenac-induced embryotoxicity and teratogenesis in Xenopus laevis and Lithobates catesbeianus, using the frog embryo teratogenesis assasy:Xenopus (FETAX)[J]. Science of The Total Environment, 2017,574:467-475.
[7]	Rozas O, Vidal C, Baeza C, et al. Organic micropollutants (OMPs) in natural waters:Oxidation by UV/H2O2treatment and toxicity assessment[J]. Water Research, 2016,98:109-118.
[8]	Espino-Estevez M R, Fernandez-Rodriguez C, Gonzalez-Diaz O M, et al. Effect of TiO2-Pd and TiO2-Ag on the photocatalytic oxidation of diclofenac, isoproturon and phenol[J]. Chemical Engineering Journal, 2016,298:82-95.
[9]	Alalm M G, Tawfik A, Ookawara S. Degradation of four pharmaceuticals by solar photo-Fenton process:Kinetics and costs estimation[J]. Journal of Environmental Chemical Engineering, 2015,3(1):46-51.
[10]	Su Y, Jassby D, Song S, et al. Enhanced oxidative and adsorptive removal of diclofenac in heterogeneous Fenton-like reaction with sulfide modified nanoscale zerovalent iron[J]. Environmental Science & Technology, 2018,52(11):6466-6475.
[11]	朱云华,朱轩墨,王旭旭,等.活性碳纤维阴极增强电-KMnO4去除水中双氯芬酸[J]. 中国环境科学, 2020,40(3):1139-1145. Zhu Y H, Zhu X M, Wang X X, et al. Removal of diclofenac in solution by activated carbon fiber cathode enhanced electro-permanganate process[J]. China Environmental Science, 2020,40(3):1139-1145.
[12]	Xian G, Zhang G, Chang H, et al. Heterogeneous activation of persulfate by Co3O4-CeO2 catalyst for diclofenac removal[J]. Journal of Environmental Management, 2019,234:265-272.
[13]	Rao Y, Zhang Y, Han F, et al. Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation:DFT-assisted mechanistic study and degradation pathways[J]. Chemical Engineering Journal, 2018,352:601-611.
[14]	史鸿乐,汪诗翔,刘义青,等.亚铁改性沸石活化过氧乙酸降解水中双氯芬酸的研究[J]. 中国环境科学, 2020,40(5):2116-2123. Shi H L, Wang S X, Liu Y Q, et al. Enhanced degradation of diclofenac by catalytic peracetic acid using Fe2+ modified zeolite[J]. China Environmental Science, 2020,40(5):2116-2123..
[15]	Hua M Y, Chen H C, Tsai R Y, et al. A novel amperometric sensor for peracetic acid based on a polybenzimidazole-modified gold electrode[J]. Electrochimica Acta, 2011,56(12):4618-4623.
[16]	Liang C, Huang C F, Chen Y J. Potential for activated persulfate degradation of BTEX contamination[J]. Water Research, 2008, 42(15):4091-4100.
[17]	Luukkonen T, Pehkonen S O. Peracids in water treatment:A critical review[J]. Critical Reviews in Environmental Science and Technology, 2017,47(1):1-39.
[18]	Wang Z, Wang J, Xiong B, et al. Application of cobalt/peracetic acid to degrade sulfamethoxazole at neutral condition:Efficiency and mechanisms[J]. Environmental Science & Technology, 2020,54(1):464-475.
[19]	Zhou F, Lu C, Yao Y, et al. Activated carbon fibers as an effective metal-free catalyst for peracetic acid activation:Implications for the removal of organic pollutants[J]. Chemical Engineering Journal, 2015,281:953-960.
[20]	Rokhina E V, Makarova K, Golovina E A, et al. Free radical reaction pathway, thermochemistry of peracetic acid homolysis, and its application for phenol degradation:Spectroscopic study and quantum chemistry calculations[J]. Environmental Science & Technology, 2010,44(17):6815-6821.
[21]	Cai M, Sun P, Zhang L, et al. UV/peracetic acid for degradation of pharmaceuticals and reactive species evaluation[J]. Environmental Science & Technology, 2017,51(24):14217-14224.
[22]	Kim J, Zhang T, Liu W, et al. Advanced oxidation process with peracetic acid and Fe (Ⅱ) for contaminant degradation[J]. Environmental Science & Technology, 2019,53(22):13312-13322.
[23]	GB/T 19104-2008过氧乙酸溶液[S]. GB/T 19104-2008 Peracetic acid solution[S].
[24]	Liu Y, He X, Fu Y, et al. Degradation kinetics and mechanism of oxytetracycline by hydroxyl radical-based advanced oxidation processes[J]. Chemical Engineering Journal, 2016,284:1317-1327.
[25]	Zhang S, Quan X, Zheng J F, et al. Probing the interphase "HO·zone" originated by carbon nanotube during catalytic ozonation[J]. Water Research, 2017,122:86-95.
[26]	Zhang L, Liu Y, Fu Y. Degradation kinetics and mechanism of diclofenac by UV/peracetic acid[J]. RSC Advances, 2020,10:9907-9916.
[27]	Shah N S, He X, Khan H M, et al. Efficient removal of endosulfan from aqueous solution by UV-C/peroxides:a comparative study[J]. Journal of Hazardous Materials, 2013,263:584-592.
[28]	Gao N, Deng Y, Zhao D. Ametryn degradation in the ultraviolet (UV) irradiation/hydrogen peroxide (H2O2) treatment[J]. Journal of Hazardous Materials, 2009,164(2/3):640-645.
[29]	Keen O S, Love N G, Linden K G. The role of effluent nitrate in trace organic chemical oxidation during UV disinfection[J]. Water Research, 2012,46(16):5224-5234.
[30]	Mack J, Bolton J R. Photochemistry of nitrite and nitrate in aqueous solution:a review[J]. Journal of Photochemistry and Photobiology A:chemistry, 1999,128(1-3):1-13.
[31]	Wu C, Linden K G. Phototransformation of selected organophosphorus pesticides:Roles of hydroxyl and carbonate radicals[J]. Water Research, 2010,44(12):3585-3594.
[32]	Canonica S, Kohn T, Mac M, et al. Photosensitizer method to determine rate constants for the reaction of carbonate radical with organic compounds[J]. Environmental Science & Technology, 2005, 39(23):9182-9188.
[33]	Dell'Arciprete M L, Soler J M, Santos-Juanes L, et al. Reactivity of neonicotinoid insecticides with carbonate radical[J]. Water Research, 2012,46(11):3479-3489.
[34]	Neta P, Huie R E, Ross A B. Rate constants for reactions of inorganic radicals in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 1988,17:1027-1284.
[35]	Huang Y, Kong M, Westerman D, et al. Effects of HCO3- on degradation of toxic contaminants of emerging concern by UV/NO3-[J]. Environmental Science & Technology, 2018,52(21):12697-12707.
[36]	Liu T, Yin K, Liu C, et al. The role of reactive oxygen species and carbonate radical in oxcarbazepine degradation via UV, UV/H2O2:Kinetics, mechanisms and toxicity evaluation[J]. Water Research, 2018,147:204-213.
[37]	Westerhoff P, Mezyk S P, Cooper W J, et al. Electron pulse radiolysis determination of hydroxyl radical rate constants with suwannee river fulvic acid and other dissolved organic matter isolates[J]. Environmental Science & Technology, 2007,41(13):4640-4646.
[38]	Mounier S, Zhao H, Garnier C, et al. Copper complexing properties of dissolved organic matter:PARAFAC treatment of fluorescence quenching[J]. Biogeochemistry, 2011,106:107-116.
[39]	李英杰,尉小旋,乔显亮,等.溶解性有机质及Cu(Ⅱ)配位对磺胺二甲基嘧啶光转化的影响[J]. 科学通报, 2015,60(30):2900-2906. Li Y J, Wei X X, Qiao X L, et al. Effects of dissolved organic matter and coordination with Cu(Ⅱ) on the phototransformation of sulfamethazine in aqueous solutions[J]. Chinese Science Bulletin, 2015,60(30):2900-2906.
[40]	Salgado R, Pereira V J, Carvalho G, et al. Photodegradation kinetics and transformation products of ketoprofen, diclofenac and atenolol in pure water and treated water[J]. Journal of Hazardous Materials, 2013,244-245:516-527.