Abstract
Solutions with 0.65 mM of the antituberculosis drug isoniazid (INH) in 0.050 M Na2SO4 at pH 3.0 were treated by electro-Fenton (EF) and UVA photoelectro-Fenton (PEF) processes using a cell with a BDD anode and a carbon-PTFE air-diffusion cathode. The influence of current density on degradation, mineralization rate, and current efficiency has been thoroughly evaluated in EF. The effect of the metallic catalyst (Fe2+ or Fe3+) and the formation of products like short-chain linear aliphatic carboxylic acids were assessed in PEF. Two consecutive pseudo-first-order kinetic regions were found using Fe2+ as catalyst. In the first region, at short time, the drug was rapidly oxidized by ●OH, whereas in the second region, at longer time, a resulting Fe(III)-INH complex was much more slowly removed by oxidants. INH disappeared completely at 300 min by EF, attaining 88 and 94% mineralization at 66.6 and 100 mA cm−2, respectively. Isonicotinamide and its hydroxylated derivative were identified as aromatic products of INH by GC-MS and oxalic, oxamic, and formic acids were quantified by ion-exclusion HPLC. The PEF treatment of a real wastewater polluted with the drug led to slower INH and TOC abatements because of the parallel destruction of its natural organic matter content.
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References
Aguilar ZG, Brillas E, Salazar M, Nava JL, Sirés I (2017) Evidence of Fenton-like reaction with active chlorine during the electrocatalytic oxidation of Acid Yellow 36 azo dye with Ir-Sn-Sb oxide anode in the presence of iron ion. Appl Catal B Environ 206:44–52. https://doi.org/10.1016/j.apcatb.2017.01.006
APHA (2012) Standard methods for the examination of water and wastewater, 22th edn. American Public Health Association, New York
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(2):2066–2075. https://doi.org/10.1016/j.jece.2016.03.012
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. https://doi.org/10.1016/j.chemosphere.2015.08.003
Brillas E, Sirés I (2015) Electrochemical removal of pharmaceuticals from water streams: reactivity elucidation by mass spectrometry. TrAC Trends Anal Chem 70:112–121. https://doi.org/10.1016/j.trac.2015.01.013
Brillas E, Calpe JC, Casado J (2000) Mineralization of 2,4-D by advanced electrochemical oxidation processes. Water Res 34(8):2253–2262. https://doi.org/10.1016/S0043-1354(99)00396-6
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. https://doi.org/10.1021/cr900136g
Flores N, Brillas E, Centellas F, Rodríguez RM, Cabot PL, Garrido JA, Sirés I (2018) Treatment of olive oil mill wastewater by single electrocoagulation with different electrodes and sequential electrocoagulation/electrochemical Fenton-based processes. J Hazard Mater 347:58–66. https://doi.org/10.1016/j.jhazmat.2017.12.059
Galia A, Lanzalaco S, Sabatino MA, Dispenza C, Scialdone O, Sirés I (2016) Crosslinking of poly(vinylpyrrolidone) activated by electrogenerated hydroxyl radicals: a first step towards a simple and cheap synthetic route of nanogel vectors. Electrochem Commun 62:64–68. https://doi.org/10.1016/j.elecom.2015.12.005
Gozzi F, Sirés I, Thiam A, Oliveira SC, Machulek Jr A, Brillas E (2017) Treatment of single and mixed pesticide formulations by solar photoelectro-Fenton using a flow plant. Chem Eng J 310:503–513. https://doi.org/10.1016/j.cej.2016.02.026
Guelfi DRV, Gozzi F, Sirés I, Brillas E, Machulek Jr A, de Oliveira SC (2017) Degradation of the insecticide propoxur by electrochemical advanced oxidation processes using a boron-doped diamond/air-diffusion cell. Environ Sci Pollut Res 24:6083–6095. https://doi.org/10.1007/s11356-016-6416-8
Guelfi DRV, Gozzi F, Machulek A Jr, Sirés I, Brillas E, de Oliveira SC (2018) Degradation of herbicide S-metolachlor by electrochemical AOPs using a boron-doped diamond anode. Catal Today. https://doi.org/10.1016/j.cattod.2017.10.026
Guevara-Almaraz E, Hinojosa-Reyes L, Caballero-Quintero A, Ruiz-Ruiz E, Hernández-Ramírez A, Guzman-Mar JL (2015) Potential of multisyringe chromatography for the on-line monitoring of the photocatalytic degradation of antituberculosis drugs in aqueous solution. Chemosphere 121:68–75. https://doi.org/10.1016/j.chemosphere.2014.11.012
Jo WK, Natarajan TS (2015a) Facile synthesis of novel redox-mediator-free direct Z-scheme CaIn2S4 marigold-flower-like/TiO2 photocatalysts with superior photocatalytic efficiency. ACS Appl Mater Interfaces 7:17138–17154. https://doi.org/10.1021/acsami.5b03935
Jo WK, Natarajan TS (2015b) Influence of TiO2 morphology on the photocatalytic efficiency of direct Z-scheme g-C3N4/TiO2 photocatalysts for isoniazid degradation. Chem Eng J 281:549–565. https://doi.org/10.1016/j.cej.2015.06.120
Kapałka A, Lanova B, Baltruschat H, Fóti G, Comninellis C (2008) Electrochemically induced mineralization of organics by molecular oxygen on boron-doped diamond electrode. Electrochem Commun 10:1215–1218. https://doi.org/10.1016/j.elecom.2008.06.005
Kapałka A, Fóti G, Comninellis C (2009) The importance of electrode material in environmental electrochemistry formation and reactivity of free hydroxyl radicals on boron-doped diamond electrodes. Electrochim Acta 54:2018–2023. https://doi.org/10.1016/j.electacta.2008.06.045
Kümmerer K (2009) Antibiotics in the aquatic environment—a review. Part I. Chemosphere 75(4):417–434. https://doi.org/10.1016/j.chemosphere.2008.11.086
Labiadh L, Barbucci A, Carpanese MP, Gadri A, Panizza M (2016) Comparative depollution of Methyl Orange aqueous solutions by electrochemical incineration using TiRuSnO2, BDD and PbO2 as high oxidation power anodes. J Electroanal Chem 766:94–99. https://doi.org/10.1016/j.jelechem.2016.01.036
Leite RMH, Leite RC, Lima JA, Foscolo CB, Mota PMPC, Lobato FCF, Lage AP (2000) HPLC identification of isoniazid residues in bovine milk. Arq Bras Med Vet Zootec 52(6):662–668. https://doi.org/10.1590/S0102-09352000000600018
Martín J, Camacho-Muñoz D, Santos JL, Aparicio I, Alonso E (2012) Occurrence of pharmaceutical compounds in wastewater and sludge from wastewater treatment plants: removal and ecotoxicological impact of wastewater discharges and sludge disposal. J Hazard Mater 239-240:40–47. https://doi.org/10.1016/j.jhazmat.2012.04.068
Martínez-Huitle CA, Rodrigo MA, Sirés I, Scialdone O (2015) Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem Rev 115:13362–13407. https://doi.org/10.1021/acs.chemrev.5b00361
Moreira FC, Boaventura RAR, Brillas E, Vilar VJP (2017) Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Appl Catal B Environ 202:217–261. https://doi.org/10.1016/j.apcatb.2016.08.037
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
Nidheesh PV, Zhou M, Oturan MA (2018) An overview on the removal of synthetic dyes from water by electrochemical advanced oxidation processes. Chemosphere 197:210–227. https://doi.org/10.1016/j.chemosphere.2017.12.195
Panizza M, Cerisola G (2009) Direct and mediated anodic oxidation of organic pollutants. Chem Rev 109:6541–6569. https://doi.org/10.1021/cr9001319
Pérez JF, Sáez C, Llanos J, Cañizares P, López C, Rodrigo MA (2017) Improving the efficiency of carbon cloth for the electrogeneration of H2O2: role of polytetrafluoroethylene and carbon black loading. Ind Eng Chem Res 56(44):12588–12595. https://doi.org/10.1021/acs.iecr.7b02563
Pullin MJ, Cabaniss SE (2003) The effects of pH, ionic strength, and iron-fulvic acid interactions on the kinetics of non-photochemical iron transformations. II. The kinetics of thermal reduction. Geochim Cosmochim Acta 67(21):4079–4089. https://doi.org/10.1016/S0016-7037(03)00367-3
Sasu S, Metzger JW, Kranert M, Kümmerer K (2015) Biodegradation of the antituberculosis drug isoniazid in the aquatic environment. Clean Soil Air Water 43(2):166–172. https://doi.org/10.1002/clen.201100147
Scior T, Meneses Morales I, Garcés Eisele SG, Domeyer D, Laufer S (2002) Antitubercular isoniazid and drug resistance of Mycobacterium tuberculosis—a review. Arch Pharm 335(11–12):511–525. https://doi.org/10.1002/ardp.200290005
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. https://doi.org/10.1016/j.envint.2011.07.012
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
Solano AMS, Garcia-Segura S, Martínez-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. Appl Catal B Environ 168-169:559–571. https://doi.org/10.1016/j.apcatb.2015.01.019
Stets S, do Amaral B, Schneider JT, de Barros IR, de Liz MV, Ribeiro RR, Nagata N, Peralta-Zamora P (2018) Antituberculosis drugs degradation by UV-based advanced oxidation processes. J Photochem Photobiol A Chem 353:26–33. https://doi.org/10.1016/j.jphotochem.2017.11.006
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
Verlicchi P, Al Aukidy M, Galletti A, Petrovic M, Barceló D (2012a) Hospital effluent: investigation of the concentrations and distribution of pharmaceuticals and environmental risk assessment. Sci Total Environ 430:109–118. https://doi.org/10.1016/j.scitotenv.2012.04.055
Verlicchi P, Al Aukidy M, Zambello E (2012b) Occurrence of pharmaceutical compounds in urban wastewater: removal, mass load and environmental risk after a secondary treatment—a review. Sci Total Environ 429:123–155. https://doi.org/10.1016/j.scitotenv.2012.04.028
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The authors thank funding from the Brazilian funding agencies: Fundação de Apoio ao Desenvolvimento do Ensino, Ciência e Tecnologia do Estado de Mato Grosso do Sul (FUNDECT-MS), Pró-Reitoria de Pesquisa e Pós-Graduação da Universidade Federal de Mato Grosso do Sul (PROPP-UFMS), Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES), and Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPQ). The authors also thank financial support from project CTQ2016-78616-R (AEI/FEDER, EU).
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Guelfi, D.R.V., Gozzi, F., Sirés, I. et al. Antituberculosis drug isoniazid degraded by electro-Fenton and photoelectro-Fenton processes using a boron-doped diamond anode and a carbon-PTFE air-diffusion cathode. Environ Sci Pollut Res 26, 4415–4425 (2019). https://doi.org/10.1007/s11356-018-2024-0
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DOI: https://doi.org/10.1007/s11356-018-2024-0