Abstract
This study is focused on the effective removal of recalcitrant pollutants hexaclorocyclohexanes (HCHs, isomers α, β, γ, and δ) and chlorobenzenes (CBs) present in a real groundwater coming from a landfill of an old lindane factory. Groundwater is characterized by a total organic carbon (TOC) content of 9 mg L−1, pH0 = 7, conductivity = 3.7 mS cm−1, high salt concentration (SO42−, HCO3−, Cl−), and ferrous iron in solution. The experiments were performed using a BDD anode and a carbon felt (CF) cathode at the natural groundwater pH and without addition of supporting electrolyte. The complete depletion of the four HCH isomers and a mineralization degree of 90% were reached at 4-h electrolysis with a current intensity of 400 mA, the residual TOC (0.8 mg L−1) corresponding mainly to formic acid. A parallel series reaction pathway was proposed: HCHs and CBs are transformed into chlorinated and hydroxylated intermediates that are rapidly oxidized to non-toxic carboxylic acids and/or mineralized, leading to a rapid decrease in solution pH.
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References
Bocos E, Oturan N, Sanromán MÁ, Oturan MA (2016) Elimination of radiocontrast agent diatrizoic acid from water by electrochemical advanced oxidation: kinetics study, mechanism and mineralization pathway. J Electroanal Chem 772:1–8. https://doi.org/10.1016/j.jelechem.2016.04.011
Brillas E, Martínez-Huitle CA (2015) Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods. An updated review. Appl Catal B-Environ 166:603–643
Brillas E, Sirés I, Oturan MA (2009) Electro-Fenton process and related electrochemical technologies based on Fenton’s reaction chemistry. Chem Rev 109(12):6570–6631. https://doi.org/10.1021/cr900136g
Buser HR, Muller MD (1995) Isomer and enantioselective degradation of hexachlorocyclohexane isomers in sewage-sludge under anaerobic conditions. Environ Sci Technol 29(3):664–672. https://doi.org/10.1021/es00003a013
Canizares P, Hernández-Ortega M, Rodrigo M, Barrera-Díaz C, Roa-Morales G, Sáez C (2009) A comparison between conductive-diamond electrochemical oxidation and other advanced oxidation processes for the treatment of synthetic melanoidins. J Hazard Mater 164(1):120–125. https://doi.org/10.1016/j.jhazmat.2008.07.134
Canizares P, Martínez L, Paz R, Saez C, Lobato J, Rodrigo MA (2006) Treatment of Fenton-refractory olive oil mill wastes by electrochemical oxidation with boron-doped diamond anodes. J Chem Technol Biot 81(8):1331–1337. https://doi.org/10.1002/jctb.1428
Chang C, Lian F, Zhu L (2011) Simultaneous adsorption and degradation of gamma-HCH by nZVI/Cu bimetallic nanoparticles with activated carbon support. Environ Pollut 159(10):2507–2514. https://doi.org/10.1016/j.envpol.2011.06.021
Criquet J, Leitner NKV (2009) Degradation of acetic acid with sulfate radical generated by persulfate ions photolysis. Chemosphere 77(2):194–200. https://doi.org/10.1016/j.chemosphere.2009.07.040
Dirany A, Efremova-Aaron S, Oturan N, Sirés I, Oturan MA, Aaron JJ (2011) Study of the toxicity of sulfamethoxazole and its degradation products in water by a bioluminescence method during application of the electro-Fenton treatment. Anal Bioanal Chem 400(2):353–360. https://doi.org/10.1007/s00216-010-4441-x
Dominguez CM, Parchão J, Rodriguez S, Lorenzo D, Romero A, Santos A (2016) Kinetics of lindane dechlorination by zero valent iron microparticles: effect of different salts and stability study. Ind Eng Chem Res 55(50):12776–12785. https://doi.org/10.1021/acs.iecr.6b03434
Elliott DW, Lien H, Zhang W (2008) Zerovalent iron nanoparticles for treatment of ground water contaminated by hexachlorocyclohexanes. J Environ Qual 37(6):2192–2201. https://doi.org/10.2134/jeq2007.0545
Fernández J, Arjol M, Cacho C (2013) POP-contaminated sites from HCH production in Sabiñánigo, Spain. Environ Sci Pollut Res 20(4):1937–1950. https://doi.org/10.1007/s11356-012-1433-8
Kesraoui-Abdessalem A, Bellakhal N, Oturan N, Dachraoui M, Oturan MA (2010) Treatment of a mixture of three pesticides by photo-and electro-Fenton processes. Desalination 250(1):450–455. https://doi.org/10.1016/j.desal.2009.09.072
Khan S, Han C, Khan HM, Boccelli DL, Dionysiou DD (2017) Efficient degradation of lindane by visible and simulated solar light-assisted S-TiO2/peroxymonosulfate process: kinetics and mechanistic investigations. J Mol Catal A-Chem 428:9–6. https://doi.org/10.1016/j.molcata.2016.11.035
Komtchou S, Dirany A, Drogui P, Bermond A (2015) Removal of carbamazepine from spiked municipal wastewater using electro-Fenton process. Environ Sci Pollut Res 22(15):11513–11525. https://doi.org/10.1007/s11356-015-4345-6
Labiadh L, Oturan MA, Panizza M, Hamadi NB, Ammar S (2015) Complete removal of AHPS synthetic dye from water using new electro-Fenton oxidation catalyzed by natural pyrite as heterogeneous catalyst. J Hazard Mater 297:34–41. https://doi.org/10.1016/j.jhazmat.2015.04.062
Madaj R, Sobiecka E, Kalinowska H (2017) Lindane, kepone and pentachlorobenzene: chloropesticides banned by Stockholm convention. Int J Environ Sci Technol:1–10. https://doi.org/10.1007/s13762-017-1417-9), https://doi.org/10.1007/s13762-017-1417-9)
Martínez-Huitle CA, Brillas E (2009) Decontamination of wastewaters containing synthetic organic dyes by electrochemical methods: a general review. Appl Catal B-Environ 87(3-4):105–145. https://doi.org/10.1016/j.apcatb.2008.09.017
Martinez-Huitle CA, Rodrigo MA, Sires I, Scialdone O (2015) Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem Rev 115(24):13362–13407. https://doi.org/10.1021/acs.chemrev.5b00361
Mascia M, Vacca A, Polcaro AM, Palmas S, Ruiz JR, Da Pozzo A (2010) Electrochemical treatment of phenolic waters in presence of chloride with boron-doped diamond (BDD) anodes: experimental study and mathematical model. J Hazard Mater 174(1-3):314–322. https://doi.org/10.1016/j.jhazmat.2009.09.053
Nidheesh PV (2015) Heterogeneous Fenton catalysts for the abatement of organic pollutants from aqueous solution: a review. RSC Adv 5(51):40552–40577. https://doi.org/10.1039/C5RA02023A
Nidheesh PV, Gandhimathi R (2012) Trends in electro-Fenton process for water and wastewater treatment: an overview. Desalination 299:1–15. https://doi.org/10.1016/j.desal.2012.05.011
Oturan MA (2000) An ecologically effective water treatment technique using electrochemically generated hydroxyl radicals for in situ destruction of organic pollutants. Application to herbicide 2,4-D. J Appl Electrochem 30:477–482
Oturan MA, Aaron JJ (2014) Advanced oxidation processes in water/wastewater treatment: principles and applications. A review. Crit Rev Environ Sci Technol 44(23):2577–2641. https://doi.org/10.1080/10643389.2013.829765
Oturan MA, Brillas E (2007) Electrochemical advanced oxidation processes (EAOPs) for environmental applications. Port Electrochim Acta 25(1):1–18. https://doi.org/10.4152/pea.200701001
Panizza M, Cerisola G (2009) Direct and mediated anodic oxidation of organic pollutants. Chem Rev 109(12):6541–6569. https://doi.org/10.1021/cr9001319
Peng L, Deng D, Guan M, Fang X, Zhu Q (2015) Remediation HCHs POPs-contaminated soil by activated persulfate technologies: feasibility, impact of activation methods and mechanistic implications. Sep Purif Technol 150:215–222. https://doi.org/10.1016/j.seppur.2015.07.002
Randazzo S, Scialdone O, Brillas E, Sirés I (2011) Comparative electrochemical treatments of two chlorinated aliphatic hydrocarbons. Time course of the main reaction by-products. J Hazard Mater 192(3):1555–1564. https://doi.org/10.1016/j.jhazmat.2011.06.075
Rodrigo MA, Oturan N, Oturan MA (2014) Electrochemically assisted remediation of pesticides in soils and water: a review. Chem Rev 114(17):8720–8745. https://doi.org/10.1021/cr500077e
Sandell EB (1959) Colorimetric determination of traces of metals. Interscience Publishers Inc., New York, Vol. 59, No. 6, p. 481
Sirés I, Brillas E, Oturan MA, Rodrigo MA, Panizza M (2014) Electrochemical advanced oxidation processes: today and tomorrow. A review. Environ Sci Pollut Res 21(14):8336–8367. https://doi.org/10.1007/s11356-014-2783-1
Sirés I, Garrido JA, Rodriguez RM, Brillas E, Oturan N, Oturan MA (2007) Catalytic behavior of the Fe+3/Fe+2 system in the electro-Fenton degradation of the antimicrobial chlorophene. Appl Catal B-Environ 72(3-4):382–394. https://doi.org/10.1016/j.apcatb.2006.11.016
Vasudevan S, Oturan MA (2014) Electrochemistry as cause and cure in water pollution. An overview. Environ Chem Lett 12(1):97–108. https://doi.org/10.1007/s10311-013-0434-2
Vega M, Romano D, Uotila E. (2016) Lindane (persistent organic pollutant) in the EU. Directorate General for Internal Policies. Policy Department C: Citizens’ Rights and Constitutional Affairs. Petitions (PETI). PE 571.398
Vijgen J (2006) The legacy of lindane HCH isomer production. Main report. International HCH & Pesticides Association, Holte, January
Vijgen J, Abhilash P, Li YF, Lal R, Forter M, Torres J, Singh N, Yunus M, Tian C, Schäffer A (2011) Hexachlorocyclohexane (HCH) as new Stockholm convention POPs—a global perspective on the management of Lindane and its waste isomers. Environ Sci Pollut Res 18(2):152–162. https://doi.org/10.1007/s11356-010-0417-9
Wacławek S, Antoš V, Hrabák P, Černík M, Elliott D (2016) Remediation of hexachlorocyclohexanes by electrochemically activated persulfates. Environ Sci Pollut Res 23(1):765–773. https://doi.org/10.1007/s11356-015-5312-y
Wang Z, Peng P, Huang W (2009) Dechlorination of gamma-hexachlorocyclohexane by zero-valent metallic iron. J Hazard Mater 166(2-3):992–997. https://doi.org/10.1016/j.jhazmat.2008.11.106
Yahya MS, Oturan N, El Kacemi K, El Karbane M, Aravindakumar CT, Oturan MA (2014) Oxidative degradation study on antimicrobial agent ciprofloxacin by electro-Fenton process: kinetics and oxidation products. Chemosphere 117:447–454. https://doi.org/10.1016/j.chemosphere.2014.08.016
Acknowledgments
The authors acknowledge Université Paris-Est Marne-la-Vallée (France) for research facilities. Carmen M. Dominguez acknowledges the Spanish MINECO for “Juan de la Cierva” post-doctoral grant (FJCI-2014-20732) and the “José Castillejo” mobility program (CAS16/00255).
Funding
The authors acknowledge financial support from Comunidad Autonoma of Madrid (Project S2013-MAE-2739 CARESOIL-CM) and from the Spanish MINECO (Project CTM2013-43794-R and CTM2016-77151-C2-1-R).
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Dominguez, C.M., Oturan, N., Romero, A. et al. Removal of organochlorine pesticides from lindane production wastes by electrochemical oxidation. Environ Sci Pollut Res 25, 34985–34994 (2018). https://doi.org/10.1007/s11356-018-1425-4
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DOI: https://doi.org/10.1007/s11356-018-1425-4