Enhanced degradation of diclofenac by catalytic peracetic acid using Fe2+ modified zeolite

SHI Hong-Le; WANG Shi-Xiang; LIU Yi-Qing; FU Yong-Sheng

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China Environmental Science ›› 2020, Vol. 40 ›› Issue (5) : 2116-2123.

Water Pollution Control

Enhanced degradation of diclofenac by catalytic peracetic acid using Fe²⁺ modified zeolite

SHI Hong-Le, WANG Shi-Xiang, LIU Yi-Qing, FU Yong-Sheng

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Abstract

A novel heterogeneous advanced oxidation system (Fe²⁺ modified zeolite/PAA) capable of generating several radicals was developed to remove diclofenac (DCF) from the contaminated water. The influences of various operational parameters including the initial pH, dosages of Fe²⁺ modified zeolite (FMZ) and PAA, as well as the water matrix on the removal of DCF were investigated. Meanwhile, the main reactive species in this system were elucidated by radical scavenging experiments. Results indicated that the DCF degradation by FMZ/PAA could be described by first-order kinetic model. DCF was completely removed in 40min under the conditions of pH 7.0, FMZ dosage of 0.2g/L, PAA dosage of 80μmol/L, initial DCF concentration of 1μmol/L and temperature of 25^oC. The presence of Cl^-, CO₃^2- and NOM had negative effects on DCF degradation through radical competition, whereas Cu²⁺ could promote obviously the DCF degradation by accelerating the activation of PAA to generate more radicals. Carbon-centered radical was proved to be mainly responsible for DCF oxidation. According to three identified products, the degradation pathway of DCF by FMZ/PAA was proposed including C-N bond cleavage, decarboxylation and formylation.

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advanced oxidation / diclofenac / ferrous ion / modified zeolite / peracetic acid

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SHI Hong-Le, WANG Shi-Xiang, LIU Yi-Qing, FU Yong-Sheng. Enhanced degradation of diclofenac by catalytic peracetic acid using Fe²⁺ modified zeolite[J]. China Environmental Science. 2020, 40(5): 2116-2123

References

[1] 夏文君,徐劼,刘锋,等.秸秆生物炭对双氯芬酸钠的吸附性能研究[J]. 中国环境科学, 2019,39(3):1054. Xia W, Xu J, Liu F, et al. Adsorption of diclofenac on straw-biochar[J]. China Environmental Science, 2019,39(3):1054.
[2] EU. Directive 2013/39/EU of the European Parliament and of the Council amending Directives 2000/60/EC and 2008/105/EC as regards priority substances in the field of water policy[J]. European Journal of Communication, 2013,226:1-17.
[3] Zhang Y J, Geissen 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] Baea S, Kimb D, Lee W. Degradation of diclofenac by pyrite catalyzed Fenton oxidation[J]. Applied Catalysis B:Environmental, 2013,134-135:93-102.
[5] Zhou T, Feng K, Zhou T, et al. Rapid decomposition of diclofenac in a magnetic field enhanced zerovalent iron/EDTA Fenton-like system[J]. Chemosphere, 2018,193:968-977.
[6] Bianchini R, Calucci L, Caretti C, et al. An EPR study on wastewater disinfection by peracetic acid, hydrogen peroxide and UV irradiation[J]. Annali di Chimica, 2002,92:783-793.
[7] Cai M, Sun P, Zhang L, et al. UV/peracetic acid for degradation of pharmaceuticals and reactive species evaluation[J]. Environmental Science & Technology, 2017,51:14217-14224.
[8] Zhang K, Zhou X, Du P, et al. Oxidation of β-lactam antibiotics by peracetic acid:Reaction kinetics, product and pathway evaluation[J]. Water Research, 2017,123:153-161.
[9] Chen S, Cai M Q, Liu Y Z, et al. Effects of water matrices on the degradation of naproxen by reactive radicals in the UV/peracetic acid process[J]. Water Research, 2019,150:153-161.
[10] Rothbart S, Embera E E, Eldik R. Mechanistic studies on the oxidative degradation of Orange II by peracetic acid catalyzed by simple manganese(II) salts. Tuning the lifetime of the catalyst[J]. New Journal of Chemistry, 2012,36:732-748.
[11] GB/T 19108-2003过氧乙酸溶液过氧乙酸含量的测定[S]. GB/T 19108-2003 Peracetic acid solution-determination of peracetic acid content[S].
[12] Ye Y C, Yang H, Wang X X, et al. Photocatalytic, Fenton and photo-Fenton degradation of RhB over Z-scheme g-C₃N₄/LaFeO₃ heterojunction photocatalysts[J]. Materials Science in Semiconductor Processing, 2018,82:14-24.
[13] Xiao R Y, Luo Z H, Wei Z S, et al. Activation of peroxymonosulfate/persulfate by nanomaterials for sulfate radical-based advanced oxidation technologies[J]. Current Opinion in Chemical Engineering, 2018,19:51-58.
[14] Yuan Z, Ni Y, Heiningen A R P. Kinetics of peracetic acid decomposition. Part I:Spontaneous decomposition at typical pulp bleaching conditions[J]. Canadian Journal of Chemical Engineering, 1997,75:37-41.
[15] Liu Y Q, He X X, Fu Y S, et al. Degradation kinetics and mechanism of oxytetracycline by hydroxyl radical-based advanced oxidation processes[J]. Chemical Engineering Journal, 2016,284:1317-1327.
[16] Liu Y Q, He X X, Duan X D, et al. Photochemical degradation of oxytetracycline:Influence of pH and role of carbonate radical[J]. Chemical Engineering Journal, 2015,276:113-121.
[17] Cope V W, Chen S N, Hoffman M Z. Intermediates in the photochemistry of carbonato-amine complexes of cobalt (III). CO₃^•- radicals and the aquocarbonato complex[J]. Journal of the American Chemical Society, 1973,95:3116-3121.
[18] Yuan R, Ramjaun S N, Wang Z, et al. Concentration profiles of chlorine radicals and their significances in ^•OH-induced dye degradation:Kinetic modeling and reaction pathways[J]. Chemical Engineering Journal, 2012,209:38-45.
[19] Kovala-Demertzi D. Transition metal complexes of diclofenac with potentially interesting anti-inflflammatory activity[J]. Journal of Inorganic Biochemistry, 2000,79:153-157.
[20] Lee E, Lee S, Lee D, et al. Lipid interaction of a-synuclein during the metal-catalyzed oxidation in the presence of Cu²⁺ and H₂O₂[J]. Journal of Neurochemistry, 2003,84:1128-1142.
[21] Vieno N M, Härkki H, Tuhkanen T, et al. Occurrence of pharmaceuticals in river water and their elimination in a pilot-scale drinking water treatment plant[J]. Environmental Science & Technology, 2007,41:5077-5084.
[22] Pham A N, Xing G, Miller C J, et al. Fenton-like copper redox chemistry revisited:hydrogen peroxide and superoxide mediation of copper-catalyzed oxidant production[J]. Journal of Catalysis, 2013, 301:54-64.
[23] Brezonik P L, Fulkerson-Brekken J. Nitrate-induced photolysis in natural waters:controls on concentrations of hydroxyl radical photo-intermediates by natural scavenging agents[J]. Environmental Science & Technology, 1998,32:3004-3010.
[24] Lipczynska-Kochany E, Kochany J. Effect of humic substances on the Fenton treatment of wastewater at acidic and neutral pH[J]. Chemosphere, 2008,73:745-750.
[25] Koivunen J and Heinonen-Tanski H. Inactivation of enteric microorganisms with chemical disinfectants, UV irradiation and combined chemical/UV treatments[J]. Water Research, 2005,39(8):1519-1526.
[26] Lubello C, Caretti C and Gori R. Comparison between PAA/UV and H₂O₂/UV disinfection for wastewater reuse[J]. Water Supply, 2002, 2(1):205-212.
[27] Buxton G V, Greenstock C L, Helman W P. Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (^•OH/^•O^-) in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 1988,17(2):513-886.
[28] 蔡美全.微量药物污染物在氯和紫外/过氧乙酸消毒过程中的降解与转化规律研究[D]. 北京:北京林业大学, 2016. Cai M. Degradation and transformation mechanisms of PhACs during chlorination and UV/peracetic acid disinfection[D]. Beijing:Beijing Forestry University, 2016.
[29] Salaeh S, Perisic D J, Biosic M, et al. Diclofenac removal by simulated solar assisted photocatalysis using TiO₂-based zeolite catalyst; mechanisms, pathways and environmental aspects[J]. Chemical Engineering Journal, 2016,304:289-302.
[30] Mugunthan E, Saidutta M B, Jagadeeshbabu P E. Photocatalytic activity of ZnO-WO₃ for diclofenac degradation under visible light irradiation[J]. Journal of Photochemistry & Photobiology A:Chemistry, 2019,383:111993.
[31] Zhao J, Liu Y, Wang Q, et al. The self-catalysis of ferrate (VI) by its reactive byproducts or reductive substances for the degradation of diclofenac:kinetics, mechanism and transformation products[J]. Separation and Purification Technology, 2018,192:412-418.
[32] Sein M, Zedd M, Tuerk J, et al. Oxidation of diclofenac with ozone in aqueous solution[J]. Environmental Science & Technology, 2008,42:6656-6662.