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Application of chemical oxidation to remediate HCH-contaminated soil under batch and flow through conditions

Abstract

This is the first study describing the chemical oxidation of hexachlorocyclohexanes (HCHs) in contaminated soil under water saturated and unsaturated flow through conditions. Soil contaminated with β-HCH (45 mg kg−1) and γ-HCH (lindane, 25 mg kg−1) was sampled from former lindane waste storage site. Efficiency of following treatments was tested at circumneutral pH: H2O2 alone, H2O2/FeII, Na2S2O8 alone, Na2S2O8/FeII, and KMnO4. Experimental conditions (oxidant dose, liquid/solid ratio, and soil granulometry) were first optimized in batch experiments. Obtained results revealed that increasing dose of H2O2 improved the oxidation efficiency while in Na2S2O8 system, maximum HCHs were removed at 300 mM. However, oxidation efficiency was slightly improved by FeII-activation. Increasing the solid/liquid ratio decreased HCH removal in soil samples crushed to 500 μm while an opposite trend was observed for 2-mm samples. Dynamic column experiments showed that oxidation efficiency followed the order KMnO4 > Na2S2O8/FeII > Na2S2O8 whatever the flow condition, whereas the removal extent declined at higher flow rate (e.g., ~50% by KMnO4 at 0.5 mL/min as compared to ~30% at 2 mL/min). Both HCH removal and oxidant decomposition extents were found higher in saturated columns than the unsaturated ones. While no significant change in relative abundance of soil mineral constituents was observed before and after chemical oxidation, more than 60% of extractable organic matter was lost after chemical oxidation, thereby underscoring the non-selective behavior of chemical oxidation in soil. Due to the complexity of soil system, chemical oxidation has rarely been reported under flow through conditions, and therefore our findings will have promising implications in developing remediation techniques under dynamic conditions closer to field applications.

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References

  1. Ahmad M, Teel AL, Watts RJ (2010) Persulfate activation by subsurface minerals. J Contam Hydrol 115:34–45

  2. Anipsitakis GP, Dionysiou DD (2004) Radical generation by the interaction of transition metals with common oxidants. Environ Sci Technol 38:3705–3712

  3. Barnes JD, Denney RC, Mendham J, Thomas MJK (2005): Analyse chimique quantitative de Vogel. De Boeck Supérieur

  4. Begum A, Gautam SK (2012) Endosulfan and lindane degradation using ozonation. Environ Technol 33:943–949

  5. Beurskens JEM, Stams AJM, Zehnder AJB, Bachmann A (1991) Relative biochemical reactivity of three hexachlorocyclohexane isomers. Ecotoxicol Environ Safety 21:128–136

  6. Brumblay RU (1971) Quantitative analysis – college outline. HarperCollins, New York

  7. Cao J, Zhang WX, Brown DG, Sethi D (2008) Oxidation of lindane with Fe (II)-activated sodium persulfate. Environ Eng Sci 25:221–228

  8. Cheng M, Zeng G, Huang D, Lai C, Xu P, Zhang C, Liu Y (2016) Hydroxyl radicals based advanced oxidation processes (AOPs) for remediation of soils contaminated with organic compounds: a review. Chem Eng J 284:582–598

  9. Dubearnes B (2006): Site de Sierentz, Etude sur les mécanismes de transfert de la pollution. Etude réalisée par l'ADEME, 32–54

  10. Hanna K, Lassabatere L, Bechet B (2012) Transport of two naphthoic acids and salicylic acid in soil: experimental study and empirical modeling. Water Res 46:4457–4467

  11. Johri AK, Dua M, Tuteja D, Saxena R, Saxena DM, Lal R (1998) Degradation of alpha, beta, gamma and delta-hexachlorocyclohexanes by Sphingomonas paucimobilis. Biotechnol Lett 20:885–887

  12. Jonsson S, Persson Y, Frankki S, van Bavel B, Lundstedt S, Haglund P, Tysklind M (2007) Degradation of polycyclic aromatic hydrocarbons (PAHs) in contaminated soils by Fenton’s reagent: a multivariate evaluation of the importance of soil characteristics and PAH properties. J Hazard Mater 149:86–96

  13. Kao CM, Huang KD, Wang JY, Chen TY, Chien HY (2008) Application of potassium permanganate as an oxidant for in situ oxidation of trichloroethylene-contaminated groundwater: a laboratory and kinetics study. J Hazard Mater 153:919–927

  14. Khan S, He X, Khan HM, Boccelli D, Dionysiou DD (2016a) Efficient degradation of lindane in aqueous solution by iron (II) and/or UV activated peroxymonosulfate. J Photochem Photobiol A 316:37–43

  15. Khan S, He X, Khan JA, Khan HM, Boccelli DL, Dionysiou DD (2016b) Kinetics and mechanism of sulfate radical- and hydroxyl radical-induced degradation of highly chlorinated pesticide lindane in UV/peroxymonosulfate system. Chem Eng J. doi:10.1016/j.cej.2016.05.150

  16. Kong SH, Watts RJ, Choi JH (1998) Treatment of petroleum-contaminated soils using iron mineral catalyzed hydrogen peroxide. Chemosphere 37:1473–1482

  17. Laurent F, Cébron A, Schwartz C, Leyval C (2012) Oxidation of a PAH polluted soil using modified Fenton reaction in unsaturated condition affects biological and physico-chemical properties. Chemosphere 86:659–664

  18. Lemaire J, Buès M, Kabeche T, Hanna K, Simonnot M-O (2013) Oxidant selection to treat an aged PAH contaminated soil by in situ chemical oxidation. J Environ Chem Eng 1:1261–1268

  19. Lewis J, Sjöstrom J (2010) Optimizing the experimental design of soil columns in saturated and unsaturated transport experiments. J Contam Hydrol 115:1–13

  20. Li S, Elliott DW, Spear ST, Ma L, Zhang W-X (2011) Hexachlorocyclohexanes in the environment: mechanisms of dechlorination. Crit Rev Environ Sci Technol 41:1747–1792

  21. Manonmani HK (2011): Bioremediation of hexachlorocyclohexane contaminated soil: field trials. Pesticides in the modern world—pesticides use and management. InTech, New York, 475-504

  22. Matta R, Hanna K, Kone T, Chiron S (2008) Oxidation of 2, 4, 6-trinitrotoluene in the presence of different iron-bearing minerals at neutral pH. Chem Eng J 144:453–458

  23. Nienow AM, Bezares-Cruz JC, Poyer IC, Hua I, Jafvert CT (2008) Hydrogen peroxide-assisted UV photodegradation of lindane. Chemosphere 72:1700–1705

  24. Nitoi I, Oncescu T, Oancea P (2013) Mechanism and kinetic study for the degradation of lindane by photo-Fenton process. J Ind Eng Chem 19:305–309

  25. Palmroth MRT, Langwaldt JH, Aunola TA, Goi A, Puhakka JA, Tuhkanen TA (2006) Treatment of PAH-contaminated soil by combination of Fenton’s reaction and biodegradation. J Chem Technol Biotech 81:598–607

  26. 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

  27. Plassard F, Winiarski T, Petit-Ramel M (2000) Retention and distribution of three heavy metals in a carbonated soil: comparison between batch and unsaturated column studies. J Contam Hydrol 42:99–111

  28. Romero A, Santos A, Vicente F, González C (2010) Diuron abatement using activated persulphate: effect of pH, Fe(II) and oxidant dosage. Chem Eng J 162:257–265

  29. Rusch B, Hanna K, Humbert B (2010) Sorption and transport of salicylate in a porous heterogeneous medium of silica quartz and goethite. Environ. Sci. Technol. 44:2447–2453

  30. Safarzadeh-Amiri A, Bolton JR, Cater SR (1996) The use of iron in advanced oxidation processes. J Adv Oxid Technol 18-26

  31. Sirguey C, Tereza de Souza e Silva P, Schwartz C, Simonnot M-O (2008) Impact of chemical oxidation on soil quality. Chemosphere 72:282–289

  32. Tamura H, Kawamura S, Hagayama M (1980) Acceleration of the oxidation of Fe2+ ions by Fe(III)-oxyhydroxides. Corros Sci 20:963–971

  33. Tseng D-H, Juang L-C, Huang H-H (2012): Effect of oxygen and hydrogen peroxide on the photocatalytic degradation of monochlorobenzene in aqueous suspension. Int. J. Photoenergy 2012

  34. Usman M, Faure P, Ruby C, Hanna K (2012a) Remediation of PAH-contaminated soils by magnetite catalyzed Fenton-like oxidation. Appl Catal B Environ 117-118:10–17

  35. Usman M, Faure P, Ruby C, Hanna K (2012b) Application of magnetite-activated persulfate oxidation for the degradation of PAHs in contaminated soils. Chemosphere 87:234–240

  36. Usman M, Tascone O, Faure P, Hanna K (2014) Chemical oxidation of hexachlorocyclohexanes (HCHs) in contaminated soils. Sci Total Environ 476-477:434–439

  37. Usman M, Hanna K, Haderlein S (2016a) Fenton oxidation to remediate PAHs in contaminated soils: a critical review of major limitations and counter-strategies. Sci Total Environ 569–570:179–190

  38. Usman M, Chaudhary A, Biache C, Faure P, Hanna K (2016b) Effect of thermal pre-treatment on the availability of PAHs for successive chemical oxidation in contaminated soils. Environ Sci Pollut Res 23:1371–1380

  39. Vijgen J, Abhilash P, Li Y, Lal R, Forter M, Torres J, Singh N, Yunus M, Tian C, Schäffer A, Weber R (2011) Hexachlorocyclohexane (HCH) as new Stockholm Convention POPs—a global perspective on the management of lindane and its waste isomers. Environ Sci Pollut Res 18:152–162

  40. Voldner EC, Li Y-F (1995) Global usage of selected persistent organochlorines. Sci Total Environ 160-161:201–210

  41. Wacławek S, Antoš V, Hrabák P, Černík M, Elliott D (2015) Remediation of hexachlorocyclohexanes by electrochemically activated persulfates. Environ Sci Pollut Res 23:765–773

  42. Wacławek S, Antoš V, Hrabák P, Černík M (2016) Remediation of hexachlorocyclohexanes by cobalt-mediated activation of peroxymonosulfate. Desalin Water Treat 57:26274–26279

  43. Wang G-S, Hsieh S-T, Hong C-S (2000) Destruction of humic acid in water by UV light—catalyzed oxidation with hydrogen peroxide. Water Res 34:3882–3887

  44. Weber JB, David MW (1982) Mobility of herbicides in soil columns under saturated- and unsaturated-flow conditions. Weed Sci 30:579–584

  45. Willett KL, Ulrich EM, Hites RA (1998) Differential toxicity and environmental fates of hexachlorocyclohexane isomers. Environ. Sci. Technol. 32:2197–2207

  46. Yan YE, Schwartz FW (1999) Oxidative degradation and kinetics of chlorinated ethylenes by potassium permanganate. J Contam Hydrol 37:343–365

  47. Zhao D, Liao X, Yan X, Huling SG, Chai T, Tao H (2013) Effect and mechanism of persulfate activated by different methods for PAHs removal in soil. J Hazard Mater 254-255:228–235

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Acknowledgments

The financial support from French organization ADEME “Agence de l'Environnement et de la Maîtrise de l'Energie” Convention no. 0972C0016 is gratefully acknowledged. The authors are also thankful to Prof. C. Ruby (UMR7564 LCPME) and C. Lorgeoux (UMR7359 Géoressources) for supporting this work.

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Correspondence to Muhammad Usman.

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Responsible editor: Philippe Garrigues

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Usman, M., Tascone, O., Rybnikova, V. et al. Application of chemical oxidation to remediate HCH-contaminated soil under batch and flow through conditions. Environ Sci Pollut Res 24, 14748–14757 (2017). https://doi.org/10.1007/s11356-017-9083-5

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Keywords

  • HCHs
  • Lindane
  • Soil remediation
  • Chemical oxidation
  • Column
  • Saturated and unsaturated conditions