Skip to main content
SpringerLink
Log in

Sequential two-column electro-Fenton-photolytic reactor for the treatment of winery wastewater

  • Advances and trends in Advanced Oxidation processes
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The high amount of winery wastewaters produced each year makes their treatment a priority issue due to their problematic characteristics such as acid pH, high concentration of organic load and colourful compounds. Furthermore, some of these effluents can have dissolved pesticides, due to the previous grape treatments, which are recalcitrant to conventional treatments. Recently, photo-electro-Fenton process has been reported as an effective procedure to mineralize different organic contaminants and a promising technology for the treatment of these complex matrixes. However, the reactors available for applying this process are scarce and they show several limitations. In this study, a sequential two-column reactor for the photo-electro-Fenton treatment was designed and evaluated for the treatment of different pesticides, pirimicarb and pyrimethanil, used in wine production. Both studied pesticides were efficiently removed, and the transformation products were determined. Finally, the treatment of a complex aqueous matrix composed by winery wastewater and the previously studied pesticides was carried out in the designed sequential reactor. The high removals of TOC and COD reached and the low energy consumption demonstrated the efficiency of this new configuration.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  • Aguera A, Almansa E, Tejedor A, Fernandez-Alba AR, Malato S, Maldonado MI (2000) Photocatalytic pilot scale degradation study of pyrimethanil and of its main degradation products in waters by means of solid-phase extraction followed by gas and liquid chromatography with mass spectrometry detection. Environ Sci Technol 34:1563–1571

    Article  Google Scholar 

  • Alfaya E, Iglesias O, Pazos M, Angeles Sanroman M (2015) Environmental application of an industrial waste as catalyst for the electro-Fenton-like treatment of organic pollutants. RSC Adv 5:14416–14424

    Article  CAS  Google Scholar 

  • Almeida LC, Silva BF, Zanoni MVB (2015) Photoelectrocatalytic/photoelectro-Fenton coupling system using a nanostructured photoanode for the oxidation of a textile dye: kinetics study and oxidation pathway. Chemosphere 136:63–71

    Article  CAS  Google Scholar 

  • Ammar S, Oturan MA, Labiadh L, Guersalli A, Abdelhedi R, Oturan N, Brillas E (2015) Degradation of tyrosol by a novel electro-Fenton process using pyrite as heterogeneous source of iron catalyst. Water Res 74:77–87

    Article  CAS  Google Scholar 

  • Aquino JM, Rocha-Filho RC, Ruotolo LAM, Bocchi N, Biaggio SR (2014) Electrochemical degradation of a real textile wastewater using β-PbO2 and DSA® anodes. Chem Eng J 251:138–145

    Article  CAS  Google Scholar 

  • Artiga P, Carballa M, Garrido JM, Mendez R (2007) Treatment of winery wastewaters in a membrane submerged bioreactor. Water Sci Technol 56:63–69

    Article  CAS  Google Scholar 

  • Barhoumi N, Labiadh L, Oturan MA, Oturan N, Gadri A, Ammar S, Brillas E (2015) Electrochemical mineralization of the antibiotic levofloxacin by electro-Fenton-pyrite process. Chemosphere 141:250–257

    Article  CAS  Google Scholar 

  • Bokare AD, Choi W (2014) Review of iron-free Fenton-like systems for activating H2O2 in advanced oxidation processes. J Hazard Mater 275:121–135

    Article  CAS  Google Scholar 

  • Bocos E, Pazos M, Angeles Sanroman M (2016) Electro-Fenton treatment of imidazolium-based ionic liquids: kinetics and degradation pathways. RSC Adv 6:1958–1965

    Article  CAS  Google Scholar 

  • Braz R, Pirra A, Lucas MS, Peres JA (2010) Combination of long term aerated storage and chemical coagulation/flocculation to winery wastewater treatment. Desalination 263:226–232

    Article  CAS  Google Scholar 

  • Brillas E, Sires I, Oturan MA (2009) Electro-Fenton process and related electrochemical technologies based on Fenton’s reaction chemistry. Chem Rev 109:6570–6631

    Article  CAS  Google Scholar 

  • Brillas E, Calpe JC, Casado J (2000) Mineralization of 2,4-D by advanced electrochemical oxidation processes. Water Res 34:2253–2262

    Article  CAS  Google Scholar 

  • Carabias-Martinez R, Garcia-Hermida U, Rodriguez-Gonzalo E, Ruano-Miguel L (2005) Behaviour of carbamate pesticides in gas chromatography and their determination with solid-phase extraction and solid-phase microextraction as preconcentration steps. J Sep Sci 28:2130–2138

    Article  CAS  Google Scholar 

  • Cesaro R (2006) PAHs and heavy metals contaminated sediment: bioavailability, mobilization, biological and phisyco-chemical treatment. Dissertation or Thesis, Università degli Studi di Napoli Federico II

  • Chen T, Tsai R, Chen Y, Huang K (2014) Electrochemical degradation of tetracycline on BDD in aqueous solutions. Int J Electrochem Sci 9:8422–8434

    CAS  Google Scholar 

  • Chen T, Fu F, Chen Z, Li D, Zhang L, Chen G (2009) Study on the photodegradation and microbiological degradation of pirimicarb insecticide by using liquid chromatography coupled with ion-trap mass spectrometry. J Chromatogr A 1216:3217–3222

    Article  CAS  Google Scholar 

  • Cihanoğlu A, Gündüz G, Dükkancı M (2015) Degradation of acetic acid by heterogeneous Fenton-like oxidation over iron-containing ZSM-5 zeolites. Appl Catal B Environ 165:687–699

    Article  Google Scholar 

  • Čuš F, Česnik HB, Bolta ŠV, Gregorčič A (2010) Pesticide residues in grapes and during vinification process. Food Control 21:1512–1518

    Article  Google Scholar 

  • de Castro Peixoto AL, Costa Teixeira AC (2014) Degradation of amicarbazone herbicide by photochemical processes. J Photochem Photobiol A 275:54–64

    Article  Google Scholar 

  • Del Real OJ, Prieto Garcia F, Santos Lopez EM, Roman Gutierrez AD, Gordillo Martinez AJ (2007) Factibility of treat wineyard wastewater through anaerobic biodigestion with a from cow's waste. Rev Tec Fac Ing Univ Zulia 30:128–135

    Google Scholar 

  • Díez AM, Iglesias O, Rosales E, Sanromán MA, Pazos M (2016) Optimization of two-chamber photo electro Fenton reactor for the treatment of winery wastewater. Process Saf Environ Prot 101:72–79

    Article  Google Scholar 

  • El-Ghenymy A, Centellas F, Maria Rodriguez R, Lluis Cabot P, Antonio Garrido J, Sires I, Brillas E (2015) Comparative use of anodic oxidation, electro-Fenton and photoelectro-Fenton with Pt or boron-doped diamond anode to decolorize and mineralize Malachite Green oxalate dye. Electrochim Acta 182:247–256

    Article  CAS  Google Scholar 

  • Fenoll J, Garrido I, Hellín P, Flores P, Vela N, Navarro S (2015) Photocatalytic oxidation of pirimicarb in aqueous slurries containing binary and ternary oxides of zinc and titanium. J Photochem Photobiol A 298:24–32

    Article  CAS  Google Scholar 

  • Forti JC, Rocha RS, Lanza MRV, Bertazzoli R (2007) Electrochemical synthesis of hydrogen peroxide on oxygen-fed graphite/PTFE electrodes modified by 2-ethylanthraquinone. J Electroanal Chem 601:63–67

    Article  CAS  Google Scholar 

  • Frontistis Z, Kouramanos M, Moraitis S, Chatzisymeon E, Hapeshi E, Fatta-Kassinos D, Xekoukoulotakis NP, Mantzavinos D (2015) UV and simulated solar photodegradation of 17α-ethynylestradiol in secondary-treated wastewater by hydrogen peroxide or iron addition. Catal Today 252:84–92

    Article  CAS  Google Scholar 

  • Garcia-Segura S, Salazar R, Brillas E (2013) Mineralization of phthalic acid by solar photoelectro-Fenton with a stirred boron-doped diamond/air-diffusion tank reactor: influence of Fe3+ and Cu2+ catalysts and identification of oxidation products. Electrochim Acta 113:609–619

    Article  CAS  Google Scholar 

  • Garza-Campos BR, Guzmán-Mar JL, Hinojosa L, Brillas E, Hernández-Ramírez A, Ruiz-Ruiz EJ (2014) Coupling of solar photoelectro-Fenton with a BDD anode and solar heterogeneous photocatalysis for the mineralization of the herbicide atrazine. Chemosphere 97:26–33

    Article  CAS  Google Scholar 

  • George SJ, Gandhimathi R, Nidheesh PV, Ramesh ST (2016) Optimization of salicylic acid removal by electro Fenton process in a continuous stirred tank reactor using response surface methodology. Desalin Water Treat 57:4234–4244

    Article  CAS  Google Scholar 

  • Gumuchian D, Cavadias S, Duten X, Tatoulian M, Da Costa P, Ognier S (2014) Organic pollutants oxidation by needle/plate plasma discharge: on the influence of the gas nature. Chem Eng Process Process Intensif 82:185–192

    Article  CAS  Google Scholar 

  • He Z, Xu Y, Wang L, Peng Y, Luo M, Cheng H, Liu X (2016) Wide-scope screening and quantification of 50 pesticides in wine by liquid chromatography/quadrupole time-of-flight mass spectrometry combined with liquid chromatography/quadrupole linear ion trap mass spectrometry. Food Chem 196:1248–1255

    Article  CAS  Google Scholar 

  • Iglesias O, Meijide J, Bocos E, Sanroman MA, Pazos M (2015) New approaches on heterogeneous electro-Fenton treatment of winery wastewater. Electrochim Acta 169:134–141

    Article  CAS  Google Scholar 

  • Ioannou LA, Puma GL, Fatta-Kassinos D (2015) Treatment of winery wastewater by physicochemical, biological and advanced processes: a review. J Hazard Mater 286:343–368

    Article  CAS  Google Scholar 

  • Ji Y, Zhou L, Ferronato C, Yang X, Salvador A, Zeng C, Chovelon J (2013) Photocatalytic degradation of atenolol in aqueous titanium dioxide suspensions: kinetics, intermediates and degradation pathways. J Photochem Photobiol A 254:35–44

    Article  CAS  Google Scholar 

  • Jimenez M, Ignacio Maldonado M, Maria Rodriguez E, Hernandez-Ramirez A, Saggioro E, Carra I, Sanchez Perez JA (2015) Supported TiO2 solar photocatalysis at semi-pilot scale: degradation of pesticides found in citrus processing industry wastewater, reactivity and influence of photogenerated species. J Chem Technol Biotechnol 90:149–157

    Article  CAS  Google Scholar 

  • Jo W, Tayade RJ (2014) New generation energy-efficient light source for photocatalysis: LEDs for environmental applications. Ind Eng Chem Res 53:2073–2084

    Article  CAS  Google Scholar 

  • Lan H, Wang A, Liu R, Liu H, Qu J (2015) Heterogeneous photo-Fenton degradation of acid red B over Fe2O3 supported on activated carbon fiber. J Hazard Mater 285:167–172

    Article  CAS  Google Scholar 

  • Li M, Qiang Z, Pulgarin C, Kiwi J (2016) Accelerated methylene blue (MB) degradation by Fenton reagent exposed to UV or VUV/UV light in an innovative micro photo-reactor. Appl Catal B Environ 187:83–89

    Article  CAS  Google Scholar 

  • Lian Y, Pang G, Shu H, Fan C, Liu Y, Feng J, Wu Y, Chang Q (2010) Simultaneous determination of 346 multiresidue pesticides in grapes by PSA-MSPD and GC-MS-SIM. J Agric Food Chem 58:9428–9453

    Article  CAS  Google Scholar 

  • Liu S, Zhao X, Sun H, Li R, Fang Y, Huang Y (2013) The degradation of tetracycline in a photo-electro-Fenton system. Chem Eng J 231:441–448

    Article  CAS  Google Scholar 

  • Lucas MS, Peres JA, Li Puma G (2010) Treatment of winery wastewater by ozone-based advanced oxidation processes (O3, O3/UV and O3/UV/H2O2) in a pilot-scale bubble column reactor and process economics. Sep Purif Technol 72:235–241

    Article  CAS  Google Scholar 

  • Marin-Benito JM, Soledad Andrades M, Sanchez-Martin MJ, Sonia Rodriguez-Cruz M (2012) Dissipation of fungicides in a vineyard soil amended with different spent mushroom substrates. J Agric Food Chem 60:6936–6945

    Article  CAS  Google Scholar 

  • Moeder M, Bauer C, Popp P, van Pinxteren M, Reemtsma T (2012) Determination of pesticide residues in wine by membrane-assisted solvent extraction and high-performance liquid chromatography-tandem mass spectrometry. Anal Bioanal Chem 403:1731–1741

    Article  CAS  Google Scholar 

  • Moreira FC, Soler J, Fonseca A, Saraiva I, Boaventura RAR, Brillas E, Vilar VJP (2016) Electrochemical advanced oxidation processes for sanitary landfill leachate remediation: evaluation of operational variables. Applied Catalysis B-Environmental 182:161–171

    Article  CAS  Google Scholar 

  • Moreira FC, Garcia-Segura S, Boaventura RAR, Brillas E, Vilar VJP (2014) Degradation of the antibiotic trimethoprim by electrochemical advanced oxidation processes using a carbon-PTFE air-diffusion cathode and a boron-doped diamond or platinum anode. Appl Catal B-Environ 160:492–505

    Article  Google Scholar 

  • Mosteo R, Sarasa J, Ormad MP, Ovelleiro JL (2008) Sequential solar photo-Fenton-biological system for the treatment of winery wastewaters. J Agric Food Chem 56:7333–7338

    Article  CAS  Google Scholar 

  • Mousset E, Frunzo L, Esposito G, van Hullebusch ED, Oturan N, Oturan MA (2016) A complete phenol oxidation pathway obtained during electro-Fenton treatment and validated by a kinetic model study. Applied Catalysis B-Environ 180:189–198

    Article  CAS  Google Scholar 

  • Muthmann R (2007) The use of plant protection products in the European Union. Data 1992–2003. Eurostat Statistical Books

  • Olvera-Vargas H, Oturan N, Oturan MA, Brillas E (2015) Electro-Fenton and solar photoelectro-Fenton treatments of the pharmaceutical ranitidine in pre-pilot flow plant scale. Sep Purif Technol 146:127–135

    Article  CAS  Google Scholar 

  • Pereira GF, El-Ghenymy A, Thiam A, Carlesi C, Eguiluz KIB, Salazar-Banda GR, Brillas E (2016) Effective removal of Orange-G azo dye from water by electro-Fenton and photoelectro-Fenton processes using a boron-doped diamond anode. Sep Purif Technol 160:145–151

    Article  CAS  Google Scholar 

  • Pirisi F, Cabras P, Garau V, Melis M, Secchi E (1996) Photodegradation of pesticides. Photolysis rates and half-life of pirimicarb and its metabolites in reactions in water and in solid phase. J Agric Food Chem 44:2417–2422

    Article  CAS  Google Scholar 

  • Remucal CK (2014) The role of indirect photochemical degradation in the environmental fate of pesticides: a review. Environmental Science-Processes & Impacts 16:628–653

    Article  CAS  Google Scholar 

  • Ribeiro AR, Nunes OC, Pereira MFR, Silva AMT (2015) An overview on the advanced oxidation processes applied for the treatment of water pollutants defined in the recently launched Directive 2013/39/EU. Environ Int 75:33–51

    Article  CAS  Google Scholar 

  • Robinson T, McMullan G, Marchant R, Nigam P (2001) Remediation of dyes in textile effluent: a critical review on current treatment technologies with a proposed alternative. Bioresour Technol 77:247–255

    Article  CAS  Google Scholar 

  • Romero E, Schmitt P, Mansour M (1994) Photolysis of pirimicarb in water under natural and simulated sunlight conditions. Pestic Sci 41:21–26

    Article  CAS  Google Scholar 

  • Romero V, Gonzalez O, Bayarri B, Marco P, Gimenez J, Esplugas S (2016) Degradation of Metoprolol by photo-Fenton: comparison of different photoreactors performance. Chem Eng J 283:639–648

    Article  CAS  Google Scholar 

  • Rosales E, Sanroman MA, Pazos M (2012) Application of central composite face-centered design and response surface methodology for the optimization of electro-Fenton decolorization of azure B dye. Environ Sci Pollut Res 19:1738–1746

    Article  CAS  Google Scholar 

  • Salazar R, Garcia-Segura S, Ureta-Zañartu MS, Brillas E (2011) Degradation of disperse azo dyes from waters by solar photoelectro-Fenton. Electrochim Acta 56:6371–6379

    Article  CAS  Google Scholar 

  • Sales Solano AM, Garcia-Segura S, Martinez-Huitle CA, Brillas E (2015) Degradation of acidic aqueous solutions of the diazo dye Congo Red by photo-assisted electrochemical processes based on Fenton's reaction chemistry. Applied Catalysis B-Environ 168:559–571

    Article  Google Scholar 

  • Salvador T, Marcolino LH Jr, Peralta-Zamora P (2012) Degradation of textile dyes and remediation of dying residues by Fenton, photo-Fenton and electro-Fenton processes. Quim Nov. 35:932–U297

  • Santana MHP, Da Silva LM, Freitas AC, Boodts JFC, Fernandes KC, De Faria LA (2009) Application of electrochemically generated ozone to the discoloration and degradation of solutions containing the dye Reactive Orange 122. J Hazard Mater 164:10–17

    Article  CAS  Google Scholar 

  • Sellers RM (1980) Spectrophotometric determination of hydrogen peroxide using potassium titanium (IV) oxalate. Analyst 105:950–954

    Article  CAS  Google Scholar 

  • Shepherd HL, Grismer ME, Tchobanoglous G (2001) Treatment of high-strength winery wastewater using a subsurface-flow constructed wetland. Water Environ Res 73:394–403

    Article  CAS  Google Scholar 

  • Shwe MT, Dimaculangan MM, de Luna MDG (2014) Decolourization of simulated dye wastewater containing reactive blue 19 (RB19) by the electro-Fenton reaction in the presence of metal oxide-coated electrodes. Frontiers in Materials and Minerals Engineering 858:40–45

    Google Scholar 

  • Silva TFCV, Ferreira R, Soares PA, Manenti DR, Fonseca A, Saraiva I, Boaventura RAR, Vilar VJP (2015) Insights into solar photo-Fenton reaction parameters in the oxidation of a sanitary landfill leachate at lab-scale. J Environ Manag 164:32–40

    Article  CAS  Google Scholar 

  • Sirtori C, Zapata A, Malato S, Agueera A (2012) Formation of chlorinated by-products during photo-Fenton degradation of pyrimethanil under saline conditions. Influence on toxicity and biodegradability. J Hazard Mater 217:217–223

    Article  Google Scholar 

  • Strong PJ (2008) Fungal remediation and subsequent methanogenic digestion of sixteen winery wastewaters. S Afr J Enol Vitic 29:85–93

    CAS  Google Scholar 

  • Szabo RK, Megyeri C, Illes E, Gajda-Schrantz K, Mazellier P, Dombi A (2011) Phototransformation of ibuprofen and ketoprofen in aqueous solutions. Chemosphere 84:1658–1663

    Article  CAS  Google Scholar 

  • Thiam A, Sires I, Brillas E (2015) Treatment of a mixture of food color additives (E122, E124 and E129) in different water matrices by UVA and solar photoelectro-Fenton. Water Res 81:178–187

    Article  CAS  Google Scholar 

  • Ting W, Lu M, Huang Y (2008) The reactor design and comparison of Fenton, electro-Fenton and photoelectro-Fenton processes for mineralization of benzene sulfonic acid (BSA). J Hazard Mater 156:421–427

    Article  CAS  Google Scholar 

  • Vaquero-Fernandez L, Sanz-Asensio J, Fernandez-Zurbano P, Lopez-Alonso M, Martinez-Soria M (2013) Determination of fungicide pyrimethanil in grapes, must, fermenting must and wine. J Sci Food Agric 93:1960–1966

    Article  CAS  Google Scholar 

  • Volmer DA (1998) Investigation of photochemical behavior of pesticides in a photolysis reactor coupled on-line with a liquid chromatography–electrospray ionization tandem mass spectrometry system: application to trace and confirmatory analyses in food samples. J Chromatography A 794:129–146

    Article  CAS  Google Scholar 

  • Vulliet E, Emmelin C, Chovelon J, Guillard C, Herrmann J (2002) Photocatalytic degradation of sulfonylurea herbicides in aqueous TiO2. Appl Catal B Environ 38:127–137

    Article  CAS  Google Scholar 

  • Wang Y, Yang B, Zhang P, Zhang W, Liu C, Shu X, Shut J (2012) Heterogeneous reactions of pirimiphos-methyl and pirimicarb with NO3 radicals. J Phys Chem A 116:10802–10809

    Article  CAS  Google Scholar 

  • Xia G, Lu Y, Xu H (2015) An energy-saving production of hydrogen peroxide via oxygen reduction for electro-Fenton using electrochemically modified polyacrylonitrile-based carbon fiber brush cathode. Sep Purif Technol 156(Part 2):553–560

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This research has been financially supported by the Xunta de Galicia and ERDF Funds (Projects CTM2014-52471-R and GRC 2013/003). The authors are grateful to the Spanish Ministry of Economy and Competitiveness for the financial support of Aida María Díez Sarabia under the FPI program and Marta Pazos under the Ramón y Cajal program.

Author information

Authors and Affiliations

  1. Department of Chemical Engineering, University of Vigo, Campus As Lagoas-Marcosende, 36310, Vigo, Spain

    A. M. Díez, M. A. Sanromán & M. Pazos

Authors
  1. A. M. Díez
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. M. A. Sanromán
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. M. Pazos
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to M. Pazos.

Additional information

Responsible editor: Bingcai Pan

Highlights

- A sequential electro-Fenton-photolytic reactor has been designed.

- The degradation of the pesticides pyrimethanil and pirimicarb has been accomplished.

- The validation of the reactor for the treatment of winery wastewater has been performed.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Díez, A.M., Sanromán, M.A. & Pazos, M. Sequential two-column electro-Fenton-photolytic reactor for the treatment of winery wastewater. Environ Sci Pollut Res 24, 1137–1151 (2017). https://doi.org/10.1007/s11356-016-7937-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-016-7937-x

Keywords

Search

Navigation