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Comparative analysis of trace contaminants in leachates before and after a pre-oxidation using a solar photo-Fenton reaction

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Abstract

Sanitary landfill leachates are a complex mixture of high-strength organic and inorganic persistent contaminants, which constitute a serious environmental problem. In this study, trace contaminants present in leachates were investigated by gas chromatography-mass spectrometry and gas chromatography-flame ionization detector before and after a pre-oxidation step using a solar photo-Fenton process. More than 40 organic compounds were detected and identified as benzene (0.09 ± 0.07 mg L-1), trichlorophenol (TCP) (0.18 ± 0.12 mg L-1), phthalate esters (Di-n-butyl phthalate (DBP), Butyl benzyl phthalate (BBP), Di(2-ethylhexyl) phthalate (DEHP)) (DBP: 0.47 ± 0.01 mg L-1; BBP: 0.36 ± 0.02 mg L-1; DEHP: 0.18 ± 0.01 mg L-1), among others. Toluene, pentachlorophenol, dimethyl phthalate, diethyl phthalate, and Di-n-octyl phthalate were never detected in any of the samples. After the photo-Fenton treatment process, TCP decreased to levels below its detection limit, benzene concentration increased approximately three times, and DBP concentration decreased about 77 % comparatively to the raw leachate sample. The solar photo-Fenton process was considered to be very efficient for the treatment of sanitary landfill leachates, leading to the complete elimination of 24 of the detected micropollutants to levels below their respective detection limits and low to significant abatement of seven other organic compounds, thus resulting in an increase of the leachate biodegradability.

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References

  • Amat AM, Arques A, Beneyto H, García A, Miranda MA, Seguí S (2003) Ozonisation coupled with biological degradation for treatment of phenolic pollutants: a mechanistically based study. Chemosphere 53:79–86

    Article  CAS  Google Scholar 

  • Bajt O, Mailhot G, Bolte M (2001) Degradation of dibutyl phthalate by homogeneous photocatalysis with Fe(III) in aqueous solution. Appl Catal B 33:239–248

    Article  CAS  Google Scholar 

  • Baun A, Ledin A, Reitzel LA, Bjerg PL, Christensen TH (2004) Xenobiotic organic compounds in leachates from ten Danish MSW landfills–chemical analysis and toxicity tests. Water Res 38:3845–3858

    Article  CAS  Google Scholar 

  • Bila D, Montalvão AF, Azevedo DA, Dezotti M (2007) Estrogenic activity removal of 17[beta]-estradiol by ozonation and identification of by-products. Chemosphere 69:736–746

    Article  CAS  Google Scholar 

  • Chen C-Y, Wu P-S, Chung Y-C (2009) Coupled biological and photo-Fenton pretreatment system for the removal of di-(2-ethylhexyl) phthalate (DEHP) from water. Bioresour Technol 100:4531–4534

    Article  CAS  Google Scholar 

  • Chipasa KB, Mdrzycka K (2008) Characterization of the fate of lipids in activated sludge. J Environ Sci 20:536–542

    Article  CAS  Google Scholar 

  • Christensen TH, Kjeldsen P, Bjerg PL, Jensen DL, Christensen JB, Baun A, Albrechtsen H-J, Heron G (2001) Biogeochemistry of landfill leachate plumes. Appl Geochem 16:659–718

    Article  CAS  Google Scholar 

  • Ciola R (1998) Fundamentals of high performance liquid chromatography – HPLC, São Paulo

  • Clesceri LS, Greenberg AE, Eaton AD, Franson MAH (1998) Standard methods for examination of water and wastewater. American Public Health Association, Washington

    Google Scholar 

  • de Morais JL, Zamora PP (2005) Use of advanced oxidation processes to improve the biodegradability of mature landfill leachates. J Hazard Mater 123:181–186

    Article  Google Scholar 

  • EMPA (1992) OECD guideline for testing of chemicals, Adopted by the Council on 17th July 1992, Zahn-wellens/EMPA test. Swiss Federal Laboratories for Materials testing and Research

  • EPA (1998) U.S. Environmental Protection Agency, Prevention, pesticides and toxic substances (7101). Fates; transport and transformation test guidelines OPPTS 835.3200 Zahn-wellens/EMPA Test. EPA 712-C-96-084, Washington, DC

  • European Commission (2000) Directive 2000/60/EC of the Council and the European Parliament of 23 October 2000 establishing a framework for community action in the field of water policy

  • Fan Y, Wang Y, Qian P-Y, Gu J-D (2004) Optimization of phthalic acid batch biodegradation and the use of modified Richards model for modelling degradation. Int Biodeterior Biodegrad 53:57–63

    Article  CAS  Google Scholar 

  • Fang C-r, Long Y-y, Shen D-s (2009) Comparison on the removal of phthalic acid diesters in a bioreactor landfill and a conventional landfill. Bioresour Technol 100:5664–5670

    Article  CAS  Google Scholar 

  • Fenton HJH (1894) Oxidation of tartaric acid in the presence of iron. J Chem Soc 65:899–910

    Article  CAS  Google Scholar 

  • Gallard H, De Laat J (2001) Kinetics of oxidation of chlorobenzenes and phenyl-ureas by Fe(II)/H2O2 and Fe(III)/H2O2. Evidence of reduction and oxidation reactions of intermediates by Fe(II) or Fe(III). Chemosphere 42:405–413

    Article  CAS  Google Scholar 

  • Gogate PR, Pandit AB (2004a) A review of imperative technologies for wastewater treatment II: hybrid methods. Adv Environ Res 8:553–597

    Article  CAS  Google Scholar 

  • Gogate PR, Pandit AB (2004b) A review of imperative technologies for wastewater treatment I: oxidation technologies at ambient conditions. Adv Environ Res 8:501–551

    Article  CAS  Google Scholar 

  • Guedes Maniero M, Maia Bila D, Dezotti M (2008) Degradation and estrogenic activity removal of 17β-estradiol and 17α-ethinylestradiol by ozonation and O3/H2O2. Sci Total Environ 407:105–115

    Article  CAS  Google Scholar 

  • Harris DC (2005) Quantitative chemical analysis, 6th edn. LTC Publisher, São Paulo

    Google Scholar 

  • Hermosilla D, Cortijo M, Huang CP (2009) Optimizing the treatment of landfill leachate by conventional Fenton and photo-Fenton processes. Sci Total Environ 407:3473–3481

    Article  CAS  Google Scholar 

  • Hongwei Y, Zhanpeng J, Shaoqi S (2004) Anaerobic biodegradability of aliphatic compounds and their quantitative structure biodegradability relationship. Sci Total Environ 322:209–219

    Article  Google Scholar 

  • Jonsson S, Ejlertsson J, Svensson BH (2003) Behaviour of mono- and diesters of o-phthalic acid in leachates released during digestion of municipal solid waste under landfill conditions. Adv Environ Res 7:429–440

    Article  CAS  Google Scholar 

  • Kaneco S, Katsumata H, Suzuki T, Ohta K (2006) Titanium dioxide mediated photocatalytic degradation of dibutyl phthalate in aqueous solution—kinetics, mineralization, and reaction mechanism. Chem Eng J 125:59–66

    Article  CAS  Google Scholar 

  • Kim S-M, Vogelpohl A (1998) Degradation of organic pollutants by the photo-Fenton process. Chem Eng Technol 21:187–191

    Article  CAS  Google Scholar 

  • Koh I-O, Chen-Hamacher X, Hicke K, Thiemann W (2004) Leachate treatment by the combination of photochemical oxidation with biological process. J Photochem Photobiol A Chem 162:261–271

    Article  CAS  Google Scholar 

  • Larson R, Bookland E, Williams R, Yocom K, Saucy D, Freeman M, Swift G (1997) Biodegradation of acrylic acid polymers and oligomers by mixed microbial communities in activated sludge. J Polym Environ 5:41–48

    CAS  Google Scholar 

  • Loureiro IR (2002) The importance and occurrence of phthalates in drinking water and in the ecosystem of the Guanabara bay. Ph.D. Thesis, Pontifícia Universidade Católica do Rio de Janeiro, Rio de Janeiro, Brazil

  • Marttinen SK, Kettunen RH, Rintala JA (2003) Occurrence and removal of organic pollutants in sewages and landfill leachates. Sci Total Environ 301:1–12

    Article  CAS  Google Scholar 

  • Méndez-Arriaga F, Esplugas S, Giménez J (2010) Degradation of the emerging contaminant ibuprofen in water by photo-Fenton. Water Res 44:589–595

    Article  Google Scholar 

  • Mrkva M (1983) Evaluation of correlations between absorbance at 254 nm and COD of rivers waters. Water Res 17:231–235

    Article  CAS  Google Scholar 

  • Nagamori M, Naruoka T, Watanabe Y, Kurata Y, Ono Y, Kawamura K (2005) Chemical characteristics of leachates in landfill sites of municipal solid wastes, Tenth International Waste Management and Landfill Symposium, Italy

  • Nascimento Filho I, von Mühlen C, Schossler P, Bastos Caramão E (2003) Identification of some plasticizers compounds in landfill leachate. Chemosphere 50:657–663

    Article  Google Scholar 

  • Nogueira RFP, Oliveira MC, Paterlini WC (2005) Simple and fast spectrophotometric determination of H2O2 in photo-Fenton reactions using metavanadate. Talanta 66:86–91

    Article  CAS  Google Scholar 

  • Nogueira RFP, Trovó AG, Silva MRA, Villa RD, Oliveira C (2007) Fundamentos e aplicações ambientais dos processos Fenton e foto-Fenton. Quim Nova 30:400–408

    Article  CAS  Google Scholar 

  • Öman CB, Junestedt C (2008) Chemical characterization of landfill leachates—400 parameters and compounds. Waste Manag (Oxf) 28:1876–1891

    Article  Google Scholar 

  • Pariente MI, Martínez F, Melero JA, Botas JÁ, Velegraki T, Xekoukoulotakis NP, Mantzavinos D (2008) Heterogeneous photo-Fenton oxidation of benzoic acid in water: effect of operating conditions, reaction by-products, and coupling with biological treatment. Appl Catal B 85:24–32

    Article  CAS  Google Scholar 

  • Queiroz SCN, Collins CH, Jardim ICSF (2001) Methods of extraction and/or concentration of compounds found in biological fluids for subsequent chromatographic determination. Quim Nova 24:68–76

    CAS  Google Scholar 

  • Rocha EMR (2010) Avaliação de sistemas de pós-tratamento de lixiviado por processos biológicos e oxidativos avançados e o desenvolvimento analítico para detecção e quantificação de compostos recalcitrantes. Ph.D. Thesis, Universidade Federal do Ceará, Fortaleza, Ceará, Brazil, 245 pp

  • Rocha EMR, Ribeiro JP, Nascimento RF, Santos AB, Mota FSB (2009) Identificação de compostos orgânicos em amostras ambientais: Aspectos metodológicos, 25º Congresso de Engenharia Sanitária e Ambiental – ABES, Recife-PE, Brazil

  • Rocha EMR, Vilar VJP, Fonseca A, Saraiva I, Boaventura RAR (2011) Landfill leachate treatment by solar-driven AOPs. Sol Energy 85:46–56

    Article  CAS  Google Scholar 

  • Salem Z, Hamouri K, Djemaa R, Allia K (2008) Evaluation of landfill leachate pollution and treatment. Desalination 220:108–114

    Article  CAS  Google Scholar 

  • Stales CA, Peterson DR, Parkerton TF, Adams WJ (1997) The environmental fate of phthalate esters: a literature review. Chemosphere 35:667–749

    Article  Google Scholar 

  • Thomas AT (2001) Analytical methods for the determination of pharmaceuticals in aqueous environmental samples. TrAC Trends Anal Chem 20:419–434

    Article  Google Scholar 

  • Torpy MF, Luthy RG, Raphaelian LA (1983) Biological oxidation of organic constituents in tar–sand combustion-process water. Biotechnol Bioeng 25:3163–3176

    Article  CAS  Google Scholar 

  • Vilar VJP, Capelo SMS, Silva TFCV, Boaventura RAR (2011a) Solar photo-Fenton as a pre-oxidation step for biological treatment of landfill leachate in a pilot plant with CPCs. Catal Today 161:228–234

    Article  CAS  Google Scholar 

  • Vilar VJP, Rocha EMR, Mota FS, Fonseca A, Saraiva I, Boaventura RAR (2011b) Treatment of a sanitary landfill leachate using combined solar photo-Fenton and biological immobilized biomass reactor at a pilot scale. Water Res 45:2647–2658

    Article  CAS  Google Scholar 

  • Vilar VJP, Moreira JMS, Fonseca A, Saraiva I, Boaventura RAR (2012a) Application of Fenton and solar photo-Fenton processes to the treatment of a sanitary landfill leachate in a pilot plant with CPCs. J Adv Oxid Technol 15:107–116

    CAS  Google Scholar 

  • Vilar VJP, Silva TFCV, Santos MAN, Fonseca A, Saraiva I, Boaventura RAR (2012b) Evaluation of solar photo-Fenton parameters on the pre-oxidation of leachates from a sanitary landfill. Sol Energy 86:3301–3315

    Article  CAS  Google Scholar 

  • Wang J, Liu P, Shi H, Qian Y (1997) Kinetics of phthalic acid ester degradation by acclimated activated sludge. Process Biochem 32:567–571

    Article  CAS  Google Scholar 

  • Wiszniowski J, Robert D, Surmacz-Gorska J, Miksch K, Weber JV (2006) Landfill leachate treatment methods: a review. Environ Chem Lett 4:51–61

    Article  CAS  Google Scholar 

  • Xu X-R, Li S-X, Li X-Y, Gu J-D, Chen F, Li X-Z, Li H-B (2009) Degradation of n-butyl benzyl phthalate using TiO2/UV. J Hazard Mater 164:527–532

    Article  CAS  Google Scholar 

  • Zhang H, Choi HJ, Huang C-P (2006) Treatment of landfill leachate by Fenton's reagent in a continuous stirred tank reactor. J Hazard Mater 136:618–623

    Article  CAS  Google Scholar 

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Acknowledgments

This work was partially supported by project PEst-C/EQB/LA0020/2011, financed by FEDER through COMPETE—Programa Operacional Factores de Competitividade, and by FCT—Fundação para a Ciência e a Tecnologia. Financial support for this work was also provided by EFACEC Ambiente SA. E. Rocha acknowledges her Ph.D. scholarship by Coord. de Aperfeiçoamento de Pessoal de Nível Superior —CAPES Process 0340/09-0. V. Vilar’s acknowledges Ciência 2008 Program.

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Correspondence to Vítor J. P. Vilar.

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Rocha, E.M.R., Mota, F.S., Vilar, V.J.P. et al. Comparative analysis of trace contaminants in leachates before and after a pre-oxidation using a solar photo-Fenton reaction. Environ Sci Pollut Res 20, 5994–6006 (2013). https://doi.org/10.1007/s11356-013-1608-y

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