Skip to main content
SpringerLink
Log in

Elimination of radiocontrast agent diatrizoic acid by photo-Fenton process and enhanced treatment by coupling with electro-Fenton process

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

The removal of radiocontrast agent diatrizoic acid (DIA) from water was performed using photo-Fenton (PF) process. First, the effect of H2O2 dosage on mineralization efficiency was determined using ultraviolet (UV) irradiation. The system reached a maximum mineralization degree of 60 % total organic carbon (TOC) removal at 4 h with 20 mM initial H2O2 concentration while further concentration values led to a decrease in TOC abatement efficiency. Then, the effect of different concentrations of Fenton’s reagents was studied for homogeneous Fenton process. Obtained results revealed that 0.25 mM Fe3+ and 20 mM H2O2 were the best conditions, achieving 80 % TOC removal efficiency at 4 h treatment. Furthermore, heterogeneous PF treatment was developed using iron-activated carbon as catalyst. It was demonstrated that this catalyst is a promising option, reaching 67 % of TOC removal within 4 h treatment without formation of iron leachate in the medium. In addition, two strategies of enhancement for process efficiency are proposed: coupling of PF with electro-Fenton (EF) process in two ways: photoelectro-Fenton (PEF) or PF followed by EF (PF-EF) treatments, achieving in both cases the complete mineralization of DIA solution within only 2 h. Finally, the Microtox tests revealed the formation of more toxic compounds than the initial DIA during PF process, while, it was possible to reach total mineralization by both proposed alternatives (PEF or PF-EF) and thus to remove the toxicity of DIA solution.

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

Similar content being viewed by others

References

  • Bañuelos JA, García-Rodríguez O, El-Ghenymy A, Rodríguez-Valadez FJ, Godínez LA, Brillas E (2016) Advanced oxidation treatment of malachite green dye using a low cost carbon-felt air-diffusion cathode. J Environ Chem Eng 4:2066–2075

    Article  Google Scholar 

  • Barreca S, Colmenares JJV, Pace A, Orecchio S, Pulgarin C (2014) Neutral solar photo-Fenton degradation of 4-nitrophenol on iron-enriched hybrid montmorillonite-alginate beads (Fe-MABs). J Photochem Photobiol A 282:33–40

    Article  CAS  Google Scholar 

  • Bocos E, Pazos M, Sanromán MA (2014) Electro-Fenton decolourization of dyes in batch mode by the use of catalytic activity of iron loaded hydrogels. J Chem Technol Biotechnol 89:1235

    Article  CAS  Google Scholar 

  • 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

    Article  CAS  Google Scholar 

  • Bouafia-Chergui S, Oturan N, Khalaf H, Oturan MA (2012) Electrochemical and photochemical oxidation of cationic dyes: a comparative study. Curr Org Chem 16:2073–2082

    Article  CAS  Google Scholar 

  • Bouafia-Chergui S, Oturan N, Khalaf H, Oturan MA (2010) Parametric study on the effect of the ratios [H2O 2]/[Fe3+] and [H2O2]/[substrate] on the photo-Fenton degradation of cationic azo dye basic blue 41. J Environ Sci Health Part A Toxic Hazard Subst Environ Eng 45:622–629

    Article  CAS  Google Scholar 

  • Brillas E, Sirés 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 (2014a) A review on the degradation of organic pollutants in waters by UV photoelectro Fenton and solar photoelectro-Fenton. J Braz Chem Soc 25:393–417

    CAS  Google Scholar 

  • Brillas E (2014b) Electro-Fenton, UVA photoelectro-Fenton and solar photoelectro-Fenton treatments of organics in waters using a boron-doped diamond anode: a review. J Mex Chem Soc 58:289–255

    Google Scholar 

  • Chiou C, Chen Y, Chang C, Chang C, Shie J, Li Y (2006) Photochemical mineralization of di-n-butyl phthalate with H2O2/Fe3+. J Hazard Mater 135:344–349

    Article  CAS  Google Scholar 

  • Daud NK, Hameed BH (2010) Fenton-like oxidation of reactive black 5 solution using iron-montmorillonite K10 catalyst. J Hazard Mater 176:1118–1121

    Article  CAS  Google Scholar 

  • Daughton CG, Ternes TA (1999) Pharmaceuticals and personal care products in the environment: agents of subtle change? Environ Health Perspect 107:907–938

    Article  CAS  Google Scholar 

  • Diagne M, Oturan N, Oturan MA, Sirés I (2009) UV-C light-enhanced photo-Fenton oxidation of methyl parathion. Environ Chem Lett 7:261–265

    Article  CAS  Google Scholar 

  • Dias IN, Souza BS, Pereira JHOS, Moreira FC, Dezotti M, Boaventura RAR, Vilar VJP (2014) Enhancement of the photo-Fenton reaction at near neutral pH through the use of ferrioxalate complexes: a case study on trimethoprim and sulfamethoxazole antibiotics removal from aqueous solutions. Chem Eng J 247:302–313

    Article  CAS  Google Scholar 

  • Dirany A, Sirés I, Oturan N, Özcan A, Oturan MA (2012) Electrochemical treatment of the antibiotic sulfachloropyridazine: kinetics, reaction pathways, and toxicity evolution. Environ Sci Technol 46:4074–4082

    Article  CAS  Google Scholar 

  • Fernández de Dios MÁ, Rosales E, Fernández-Fernández M, Pazos M, Sanromán MÁ (2015) Degradation of organic pollutants by heterogeneous electro-Fenton process using Mn-alginate composite. J Chem Technol Biotechnol 90:1439–1447

    Article  Google Scholar 

  • Florenza X, Solano AMS, Centellas F, Martínez-Huitle CA, Brillas E, Garcia-Segura S (2015) Degradation of the azo dye acid red 1 by anodic oxidation and indirect electrochemical processes based on Fenton’s reaction chemistry. Relationship between decolorization, mineralization and products. Electrochim Acta 142:276–288

    Article  Google Scholar 

  • Florenza X, Garcia-Segura S, Centellas F, Brillas E (2016)  Comparative electrochemical degradation of salicylic and aminosalicylic acids: influence of functional groups on decay kinetics and mineralization. Chemosphere 154:171–178

  • Foo KY, Hameed BH (2009) An overview of landfill leachate treatment via activated carbon adsorption process. J Hazard Mater 171:54–60

    Article  CAS  Google Scholar 

  • García-Rodríguez O, Bañuelos JA, El-Ghenymy A, Godínez LA, Brillas E, Rodríguez-Valadez FJ (2016) Use of a carbon felt–iron oxide air-diffusion cathode for the mineralization of malachite green dye by heterogeneous electro-Fenton and UVA photoelectro-Fenton processes. J Electroanal Chem 767:40–48

    Article  Google Scholar 

  • Garcia-Segura S, Brillas E (2011) Mineralization of the recalcitrant oxalic and oxamic acids by electrochemical advanced oxidation processes using a boron-doped diamond anode. Water Res 45:2975–2984

    Article  CAS  Google Scholar 

  • Garcia-Segura S, El-Ghenymy A, Centellas F, Rodríguez RM, Arias C, Garrido JA, Cabot PL, Brillas E (2012) Comparative degradation of the diazo dye direct yellow 4 by electro-Fenton, photoelectro-Fenton and photo-assisted electro-Fenton. J Electroanal Chem 681:36–43

    Article  CAS  Google Scholar 

  • Garcia-Segura S, Brillas E, Cornejo-Ponce L, Salazar R (2016) Effect of the Fe3+/Cu2+ ratio on the removal of the recalcitrant oxalic and oxamic acids by electro-Fenton and solar photoelectro-Fenton, Sol. Energy 124:242–253

    CAS  Google Scholar 

  • Ghaly MY, Härtel G, Mayer R, Haseneder R (2001) Photochemical oxidation of p-chlorophenol by UV/H2O2 and photo-Fenton process. A comparative study. Waste Manag 21:41–47

    Article  CAS  Google Scholar 

  • Gur-Reznik S, Azerrad SP, Levinson Y, Heller-Grossman L, Dosoretz CG (2011) Iodinated contrast media oxidation by nonthermal plasma: the role of iodine as a tracer. Water Res 45:5047–5057

    Article  CAS  Google Scholar 

  • Hammouda SB, Adhoum N, Monser L (2015) Synthesis of magnetic alginate beads based on Fe3O4 nanoparticles for the removal of 3-methylindole from aqueous solution using Fenton process. J Hazard Mater 294:128–136

    Article  CAS  Google Scholar 

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

    Article  CAS  Google Scholar 

  • Iglesias O, Gómez J, Pazos M, Sanromán MA (2014) Electro-Fenton oxidation of imidacloprid by Fe alginate gel beads. Appl Catal B Environ 144:416–424

    Article  CAS  Google Scholar 

  • Iglesias O, Fernández de Dios MA, Pazos M, Sanromán MA (2013) Using iron-loaded sepiolite obtained by adsorption as a catalyst in the electro-Fenton oxidation of reactive black 5. Environ Sci Pollut Res 20:5983–5993

    Article  CAS  Google Scholar 

  • Karthikeyan S, Sekaran G (2014) In situ generation of a hydroxyl radical by nanoporous activated carbon derived from rice husk for environmental applications: kinetic and thermodynamic constants. Phys Chem Chem Phys 16:3924–3933

    Article  CAS  Google Scholar 

  • Krzeminska D, Neczaj E, Borowski G (2015) Advanced oxidation processes for food industrial wastewater decontamination. J Ecol Eng 16:61–71

    Article  Google Scholar 

  • Laurencé C, Rivard M, Thierry M, Morin C, Buisson D, Bourcier S, Sablier M, Oturan MA (2014) Reinvestigation of the oxidative metabolic pathways of furosemide and identification of a toxic metabolite. Chemosphere 113:193–199

    Article  Google Scholar 

  • Loaiza-Ambuludi S, Panizza M, Oturan N, Oturan MA (2014) Removal of the anti-inflammatory drug ibuprofen from water using homogeneous photocatalysis. Catal Today 224:29–33

    Article  CAS  Google Scholar 

  • Malato S (2008) Removal of emerging contaminants in waste-water treatment: Removal by photo-catalytic processes. Handb Environ Chem Vol 5 Water Pollut 5(S2):177–197

  • Moreira FC, Garcia-Segura S, Vilar VJP, Boaventura RAR, Brillas E (2013) Decolorization and mineralization of sunset yellow FCF azo dye by anodic oxidation, electro-Fenton, UVA photoelectro-Fenton and solar photoelectro-Fenton processes. Appl Catal B Environ 142-143:877–890

    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 160-161:492–505

    Article  CAS  Google Scholar 

  • Murgolo S, Petronella F, Ciannarella R, Comparelli R, Agostiano A, Curri ML, Mascolo G (2015) UV and solar-based photocatalytic degradation of organic pollutants by nano-sized TiO2 grown on carbon nanotubes. Catal Today 240:114–124

    Article  CAS  Google Scholar 

  • Neyens E, Baeyens J (2003) A review of classic Fenton’s peroxidation as an advanced oxidation technique. J Hazard Mater 98:33–50

    Article  CAS  Google Scholar 

  • Oh SY, Yoon HS, Jeong TY, Kim SD (2015) Evaluation of remediation processes for explosive-contaminated soils: kinetics and Microtox® bioassay. J Chem Technol Biotechnol 91:928–937

    Article  Google Scholar 

  • Oturan N, Trajkovska S, Oturan MA, Couderchet M, Aaron JJ (2008) Study of the toxicity of diuron and its metabolites formed in aqueous medium during application of the electrochemical advanced oxidation process “electro-Fenton”. Chemosphere 73:1550–1556

    Article  CAS  Google Scholar 

  • Oturan N, Brillas E, Oturan MA (2012) Unprecedented total mineralization of atrazine and cyanuric acid by anodic oxidation and electro-Fenton with a boron-doped diamond anode. Environ Chem Lett 10:165–170

    Article  CAS  Google Scholar 

  • Oturan MA, Aaron J-J (2014) Advanced oxidation processes in water/wastewater treatment: principles and applications. A review. Crit Rev Environ Sci Technol 44:2577–2641

    Article  CAS  Google Scholar 

  • Papoutsakis S, Afshari Z, Malato S, Pulgarin C (2015) Elimination of the iodinated contrast agent iohexol in water, wastewater and urine matrices by application of photo-Fenton and ultrasound advanced oxidation processes. J Environ Chem Eng 3:2002–2009

    Article  CAS  Google Scholar 

  • Pignatello JJ, Oliveros E, MacKay A (2006) Advanced oxidation processes for organic contaminant destruction based on the Fenton reaction and related chemistry. Crit Rev Environ Sci Technol 36:1–84

    Article  CAS  Google Scholar 

  • Pignatello JJ, Sun Y (1995) Complete oxidation of metolachlor and methyl parathion in water by the photoassisted Fenton reaction. Water Res 29:1837–1844

    Article  CAS  Google Scholar 

  • Plewa MJ, Muellner MG, Richardson SD, Fasano F, Buettner KM, Woo Y, Mckague AB, Wagner ED (2008) Occurrence, synthesis, and mammalian cell cytotoxicity and genotoxicity of haloacetamides: an emerging class of nitrogenous drinking water disinfection byproducts. Environ Sci Technol 42:955–961

    Article  CAS  Google Scholar 

  • Radjenovic J, Flexer V, Donose BC, Sedlak DL, Keller J (2013) Removal of the X-ray contrast media diatrizoate by electrochemical reduction and oxidation. Environ Sci Technol 47:13686–13694

    Article  CAS  Google Scholar 

  • Rastogi T, Leder C, Kümmerer K (2014) Qualitative environmental risk assessment of photolytic transformation products of iodinated X-ray contrast agent diatrizoic acid. Sci Total Environ 482-483:378–388

    Article  CAS  Google Scholar 

  • Real FJ, Javier Benitez F, Acero JL, Sagasti JJP, Casas F (2009) Kinetics of the chemical oxidation of the pharmaceuticals primidone, ketoprofen, and diatrizoate in ultrapure and natural waters. Ind Eng Chem Res 48:3380–3388

    Article  CAS  Google Scholar 

  • Richardson SD, Fasano F, Ellington JJ, Crumley FG, Buettner KM, Evans JJ, Blount BC, Silva LK, Waite TJ, Luther GW, Mckague AB, Miltner RJ, Wagner ED, Plewa MJ (2008) Occurrence and mammalian cell toxicity of iodinated disinfection byproducts in drinking water. Environ Sci Technol 42:8330–8338

    Article  CAS  Google Scholar 

  • Rosales E, Iglesias O, Pazos M, Sanromán MA (2012) Decolourisation of dyes under electro-Fenton process using Fe alginate gel beads. J Hazard Mater 213-214:369–377

    Article  CAS  Google Scholar 

  • Rubio-Clemente A, Chica Arrieta EL, Peñuela Mesa GA (2013) Wastewater treatment processes for the removal of emerging organic pollutants. Rev Ambiente Agua 8:93–103

    Google Scholar 

  • Rubio-Clemente A, Chica E, Peñuela GA (2015) Petrochemical wastewater treatment by photo-Fenton process. Water Air Soil Pollut 226. doi:10.1007/s11270-015-2321-x

  • Russo AV, Toriggia LF, Jacobo SE (2014) Natural clinoptilolite-zeolite loaded with iron for aromatic hydrocarbons removal from aqueous solutions. J Mater Sci 49:614–620

    Article  CAS  Google Scholar 

  • Sedaghat M, Vahid B, Aber S, Rasoulifard MH, Khataee A, Daneshvar N (2016) Electrochemical and photo-assisted electrochemical treatment of the pesticide imidacloprid in aqueous solution by the Fenton process: effect of operational parameters. Res Chem Intermed 42:855–868

    Article  CAS  Google Scholar 

  • Sirés I, Brillas E (2012) Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies: a review. Environ Int 40:212–229

    Article  Google Scholar 

  • Sirés I, Brillas E, Oturan MA, Rodrigo MA, Panizza M (2014) Electrochemical advanced oxidation processes: today and tomorrow. A review. Environ Sci Pollut Res 8336–8367.

  • Stüber F, Font J, Fortuny A, Bengoa C, Eftaxias A, Fabregat A (2005) Carbon materials and catalytic wet air oxidation of organic pollutants in wastewater. Top Catal 33:3–50

    Article  Google Scholar 

  • Stumm-Zollinger E, Fair GM (1965) Biodegradation of steroid hormones. J Water Pollut Control Fed 37:1506–1510

    CAS  Google Scholar 

  • Ternes TA, Stüber J, Herrmann N, McDowell D, Ried A, Kampmann M, Teiser B (2003) Ozonation: a tool for removal of pharmaceuticals, contrast media and musk fragrances from wastewater? Water Res 37:1976–1982

    Article  CAS  Google Scholar 

  • Tiehm A, Schmidt N, Stieber M, Sacher F, Wolf L, Hoetzl H (2011) Biodegradation of Phmaceutical compounds and their occurrence in the Jordan Valley. Water Resour Manag 25:1195–1203

    Article  Google Scholar 

  • Umar M, Aziz HA, Yusoff MS (2010) Trends in the use of Fenton, electro-Fenton and photo-Fenton for the treatment of landfill leachate. Waste Manag 30:2113–2121

    Article  CAS  Google Scholar 

  • Velo-Gala I, López-Peñalver JJ, Sánchez-Polo M, Rivera-Utrilla J (2012) Ionic X-ray contrast media degradation in aqueous solution induced by gamma radiation. Chem Eng J 195–196:369–376

    Article  Google Scholar 

  • Velo-Gala I, López-Peñalver JJ, Sánchez-Polo M, Rivera-Utrilla J (2014) Comparative study of oxidative degradation of sodium diatrizoate in aqueous solution by H2O2/Fe2+, H2O2/Fe3+, Fe (VI) and UV, H2O2/UV, K2S2O8/UV. Chem Eng J 241:504–512

    Article  CAS  Google Scholar 

  • Xu P, Han H, Zhuang H, Hou B, Jia S, Xu C, Wang D (2015) Advanced treatment of biologically pretreated coal gasification wastewater by a novel integration of heterogeneous Fenton oxidation and biological process. Bioresour Technol 182:389–392

    Article  CAS  Google Scholar 

  • Zhao C, Arroyo-Mora LE, DeCaprio AP, Sharma VK, Dionysiou DD, O’Shea KE (2014) Reductive and oxidative degradation of iopamidol, iodinated X-ray contrast media, by Fe(III)-oxalate under UV and visible light treatment. Water Res 67:144–153

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This research has been financially supported by the Spanish Ministry of Economy and Competitiveness and ERDF Funds (Projects CTM2014-52471-R). The authors are grateful to the Spanish Ministry of Economy and Competitiveness for the financial support of Elvira Bocos under the FPI programme and the mobility grant: EEBB-I-14-09087.

Author information

Authors and Affiliations

  1. Department of Chemical Engineering, University of Vigo, Isaac Newton Building, Campus As Lagoas Marcosende, 36310, Vigo, Spain

    Elvira Bocos, Marta Pazos & M. Ángeles Sanromán

  2. Laboratoire Géomatériaux et Environnement (LGE), Université Paris-Est, EA 4508, 77454, Marne-la-Vallée, France

    Elvira Bocos, Nihal Oturan & Mehmet A. Oturan

Authors
  1. Elvira Bocos
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Nihal Oturan
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Marta Pazos
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. M. Ángeles Sanromán
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Mehmet A. Oturan
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Mehmet A. Oturan.

Additional information

Responsible editor: Vítor Pais Vilar

Highlights

• Optimization of key parameters in photo-Fenton (PF) removal of diatrizoic acid (DIA)

• Eighty per cent TOC removal under homogeneous PF using 0.25 mM Fe3+ and 20 mM H2O2

• Sixty-seven per cent TOC removal under heterogeneous PF using iron-activated carbon

• Complete mineralization by photoelectro-Fenton (PEF) or PF followed by EF process (PF-EF)

• Removal of the toxicity of DIA solution by PEF or PF-EF

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Bocos, E., Oturan, N., Pazos, M. et al. Elimination of radiocontrast agent diatrizoic acid by photo-Fenton process and enhanced treatment by coupling with electro-Fenton process. Environ Sci Pollut Res 23, 19134–19144 (2016). https://doi.org/10.1007/s11356-016-7054-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-016-7054-x

Keywords

Search

Navigation