Efficient removal of diuretic hydrochlorothiazide from water by electro-Fenton process using BDD anode: a kinetic and degradation pathway study
Hélène Monteil A , Nihal Oturan A , Yoan Péchaud A and Mehmet A. Oturan A BA Université Paris-Est, Laboratoire Géomatériaux et Environnement (EA 4508), UPEM, 5 Bd Descartes, 77454 Marne-la-Vallée, Cedex 2, France.
B Corresponding author. Email: mehmet.oturan@univ-paris-est.fr
Environmental Chemistry 16(8) 613-621 https://doi.org/10.1071/EN19121
Submitted: 29 April 2019 Accepted: 25 June 2019 Published: 24 July 2019
Environmental context. Hydrochlorothiazide, a common diuretic pharmaceutical, occurs in environmental waters because current treatment technologies are unable to eliminate it from wastewater. To remove this environmentally hazardous chemical from water, we developed an advanced electrochemical oxidation process to efficiently degrade and mineralise the compound. Wider application of the process holds the promise of general, efficient destruction of pharmaceuticals in aqueous media.
Abstract. The degradation and the mineralisation of the diuretic hydrochlorothiazide were studied by an advanced electrochemical oxidation process, ‘electro-Fenton’, which generates in situ hydroxyl radicals that are able to successfully oxidise or mineralise organic pollutants. In this study, a 0.1 mM (29.8 mg L−1) hydrochlorothiazide solution was completely oxidatively degraded in 15 min under constant current electrolysis at 500 mA. The absolute kinetic rate constant of the oxidation reaction was also determined as (4.37 ± 0.04) × 109 M−1 s−1. The quasi-complete mineralisation of the solution was obtained with electrolysis for 6 h under the same applied current. Several oxidation reaction intermediates were identified using gas chromatography-mass spectrometry (GC-MS). The formed carboxylic acids during the mineralisation process were also studied; oxamic, oxalic, acetic and maleic acids were identified and their concentrations were monitored throughout the electrolysis. The ions released during the treatment were also considered. Based on these data and the total organic carbon (TOC) removal results, a possible mineralisation pathway was proposed. These findings enable the conclusion that the electro-Fenton process is an efficient and environmentally-friendly method to eliminate the hazardous drug hydrochlorothiazide from an aqueous environment.
Additional keywords: hydroxyl radicals, mineralisation, wastewater treatment.
References
Bellakhal N, Oturan MA, Oturan N, Dachraoui M (2006). Olive Oil Mill Wastewater Treatment by the electro-Fenton Process. Environmental Chemistry 3, 345–349.| Olive Oil Mill Wastewater Treatment by the electro-Fenton ProcessCrossref | GoogleScholarGoogle Scholar |
Borowska E, Bourgin M, Hollender J, Kienle C, McArdell CS, von Gunten U (2016). Oxidation of cetirizine, fexofenadine and hydrochlorothiazide during ozonation: Kinetics and formation of transformation products. Water Research 94, 350–362.
| Oxidation of cetirizine, fexofenadine and hydrochlorothiazide during ozonation: Kinetics and formation of transformation productsCrossref | GoogleScholarGoogle Scholar | 26971810PubMed |
Bouissou-Schurtz C, Houeto P, Guerbet M, Bachelot M, Casellas C, Mauclaire A-C, Panetier P, Delval C, Masset D (2014). Ecological risk assessment of the presence of pharmaceutical residues in a French national water survey. Regulatory Toxicology and Pharmacology 69, 296–303.
| Ecological risk assessment of the presence of pharmaceutical residues in a French national water surveyCrossref | GoogleScholarGoogle Scholar | 24768990PubMed |
Boxall ABA (2004). The environmental side effects of medication. EMBO Reports 5, 1110–1116.
| The environmental side effects of medicationCrossref | GoogleScholarGoogle Scholar |
Brillas E, Sirés I, Oturan MA (2009). Electro-fenton process and related electrochemical technologies based on fenton’s reaction chemistry. Chemical Reviews 109, 6570–6631.
| Electro-fenton process and related electrochemical technologies based on fenton’s reaction chemistryCrossref | GoogleScholarGoogle Scholar | 19839579PubMed |
Brito C do N, de Araújo DM, Martínez-Huitle CA, Rodrigo MA (2015). Understanding active chlorine species production using boron doped diamond films with lower and higher sp3/sp2 ratio. Electrochemistry Communications 55, 34–38.
| Understanding active chlorine species production using boron doped diamond films with lower and higher sp3/sp2 ratioCrossref | GoogleScholarGoogle Scholar |
Buxton GV, Greenstock CL, Helman WP, Ross AB (1988). Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (OH/O−) in aqueous solution. Journal of Physical and Chemical Reference Data 17, 513–886.
| Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (OH/O−) in aqueous solutionCrossref | OH/O−) in aqueous solution&journal=Journal of Physical and Chemical Reference Data&volume=17&pages=513-886&publication_year=1988&author=GV%20Buxton&hl=en&doi=10.1063/1.555805" target="_blank" rel="nofollow noopener noreferrer" class="reftools">GoogleScholarGoogle Scholar |
Dirany A, Sirés I, Oturan N, Özcan A, Oturan MA (2012). Electrochemical treatment of the antibiotic sulfachloropyridazine: kinetics, reaction pathways, and toxicity evolution. Environmental Science & Technology 46, 4074–4082.
| Electrochemical treatment of the antibiotic sulfachloropyridazine: kinetics, reaction pathways, and toxicity evolutionCrossref | GoogleScholarGoogle Scholar |
Dominguez CM, Oturan N, Romero A, Santos A, Oturan MA (2018). Optimization of electro-Fenton process for effective degradation of organochlorine pesticide lindane. Catalysis Today 313, 196–202.
| Optimization of electro-Fenton process for effective degradation of organochlorine pesticide lindaneCrossref | GoogleScholarGoogle Scholar |
Faouzi M, Cañizares P, Gadri A, Lobato J, Nasr B, Paz R, Rodrigo MA, Saez C (2006). Advanced oxidation processes for the treatment of wastes polluted with azoic dyes. Electrochimica Acta 52, 325–331.
| Advanced oxidation processes for the treatment of wastes polluted with azoic dyesCrossref | GoogleScholarGoogle Scholar |
Fernández C, González-Doncel M, Pro J, Carbonell G, Tarazona JV (2010). Occurrence of pharmaceutically active compounds in surface waters of the Henares-Jarama-Tajo river system (Madrid, Spain) and a potential risk characterization. The Science of the Total Environment 408, 543–551.
| Occurrence of pharmaceutically active compounds in surface waters of the Henares-Jarama-Tajo river system (Madrid, Spain) and a potential risk characterizationCrossref | GoogleScholarGoogle Scholar | 19889447PubMed |
Ganiyu SO, Le TXH, Bechelany M, Oturan N, Papirio S, Esposito E, Hullebusch EV, Cretin M, Oturan MA (2018). Electrochemical mineralization of sulfamethoxazole over wide pH range using FeII/FeIII LDH modified carbon felt cathode: Degradation pathway, toxicity and reusability of the modified cathode. Chemical Engineering Journal 350, 844–855.
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 Research 45, 2975–2984.
| Mineralization of the recalcitrant oxalic and oxamic acids by electrochemical advanced oxidation processes using a boron-doped diamond anodeCrossref | GoogleScholarGoogle Scholar | 21477836PubMed |
Garcia-Segura S, Lanzarini-Lopes M, Hristovski K, Westerhoff P (2018). Electrocatalytic reduction of nitrate: Fundamentals to full-scale water treatment applications. Applied Catalysis B: Environmental 236, 546–568.
| Electrocatalytic reduction of nitrate: Fundamentals to full-scale water treatment applicationsCrossref | GoogleScholarGoogle Scholar |
Jones OAH, Voulvoulis N, Lester JN (2005). Human pharmaceuticals in wastewater treatment processes. Critical Reviews in Environmental Science and Technology 35, 401–427.
| Human pharmaceuticals in wastewater treatment processesCrossref | GoogleScholarGoogle Scholar |
Kabdasli I, Olmez-Hanci T, Akgun G, Tunay O (2019). Assessment of pollution profile ans wastewater control alternatives of a pharmaceutical industry. Fresenius Environmental Bulletin 28, 516–522.
Khetan KS, Collins JT (2007). Human pharmaceuticals in the aquatic environment: a challenge to green chemistry. Chemical Reviews 107, 2319–2364.
| Human pharmaceuticals in the aquatic environment: a challenge to green chemistryCrossref | GoogleScholarGoogle Scholar |
Klavarioti M, Mantzavinos D, Kassinos D (2009). Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processes. Environment International 35, 402–417.
| Removal of residual pharmaceuticals from aqueous systems by advanced oxidation processesCrossref | GoogleScholarGoogle Scholar | 18760478PubMed |
Kremer ML (2003). The Fenton Reaction. Dependence of the Rate on pH. The Journal of Physical Chemistry A 107, 1734–1741.
| The Fenton Reaction. Dependence of the Rate on pHCrossref | GoogleScholarGoogle Scholar |
Küster A, Adler N (2014). Pharmaceuticals in the environment: scientific evidence of risks and its regulation. Philosophical Transactions of the Royal Society B 369, 20130587
Lindsey ME, Meyer M, Thurman EM (2001). Analysis of trace levels of sulfonamide and tetracycline antimicrobials in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometry. Analytical Chemistry 73, 4640–4646.
| Analysis of trace levels of sulfonamide and tetracycline antimicrobials in groundwater and surface water using solid-phase extraction and liquid chromatography/mass spectrometryCrossref | GoogleScholarGoogle Scholar | 11605842PubMed |
Luo Y, Guo W, Ngo HH, Nghiem LD, Hai FI, Zhang J, Liang S, Wang XC (2014). A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatment. The Science of the Total Environment 473–474, 619–641.
| A review on the occurrence of micropollutants in the aquatic environment and their fate and removal during wastewater treatmentCrossref | GoogleScholarGoogle Scholar | 24394371PubMed |
Marcelino RBP, Andrade LN, Starling MCVM, Amorim CC, Barbosa MLT, Lopes RP, Reis BG, Leão MMD (2016). Evaluation of aerobic and anaerobic biodegradability and toxicity assessment of real pharmaceutical wastewater from industrial production of antibiotics. Brazilian Journal of Chemical Engineering 33, 445–452.
| Evaluation of aerobic and anaerobic biodegradability and toxicity assessment of real pharmaceutical wastewater from industrial production of antibioticsCrossref | GoogleScholarGoogle Scholar |
Margot J, Rossi L, Barry DA, Holliger C (2015). A review of the fate of micropollutants in wastewater treatment plants. WIREs. Water 2, 457–487.
| A review of the fate of micropollutants in wastewater treatment plantsCrossref | GoogleScholarGoogle Scholar |
Martin de Vidales MJ, Millan M, Saez C, Cañizares P, Rodrigo MA (2016). What happens to inorganic nitrogen species during conductive diamond electrochemical oxidation of real wastewater?. Electrochemistry Communications 67, 65–68.
| What happens to inorganic nitrogen species during conductive diamond electrochemical oxidation of real wastewater?Crossref | GoogleScholarGoogle Scholar |
Mendoza A, Aceña J, Pérez S, López de Alda M, Barceló D, Gil A, Valcárcel Y (2015). Pharmaceuticals and iodinated contrast media in a hospital wastewater: a case study to analyse their presence and characterise their environmental risk and hazard. Environmental Research 140, 225–241.
| Pharmaceuticals and iodinated contrast media in a hospital wastewater: a case study to analyse their presence and characterise their environmental risk and hazardCrossref | GoogleScholarGoogle Scholar | 25880605PubMed |
Monteil H, Péchaud Y, Oturan N, Oturan MA (2019). A review on efficiency and cost effectiveness of electro- and bio-electro-Fenton processes: application to the treatment of pharmaceutical pollutants in water. Chemical Engineering Journal
| A review on efficiency and cost effectiveness of electro- and bio-electro-Fenton processes: application to the treatment of pharmaceutical pollutants in waterCrossref | GoogleScholarGoogle Scholar | in press
Mousset E, Wang Z, Hammaker J, Lefebvre O (2016). Physico-chemical properties of pristine graphene and its performance as electrode material for electro-Fenton treatment of wastewater. Electrochimica Acta 214, 217–230.
| Physico-chemical properties of pristine graphene and its performance as electrode material for electro-Fenton treatment of wastewaterCrossref | GoogleScholarGoogle Scholar |
Mousset E, Oturan N, Oturan MA (2018). An unprecedented route of OH radical reactivity evidenced by an electrocatalytical process: Ipso-substitution with perhalogenocarbon compounds. Applied Catalysis B: Environmental 226, 135–146.
| An unprecedented route of OH radical reactivity evidenced by an electrocatalytical process: Ipso-substitution with perhalogenocarbon compoundsCrossref | GoogleScholarGoogle Scholar |
Nidheesh PV, Gandhimathi R (2012). Trends in electro-Fenton process for water and wastewater treatment: an overview. Desalination 299, 1–15.
| Trends in electro-Fenton process for water and wastewater treatment: an overviewCrossref | GoogleScholarGoogle Scholar |
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.
Nidheesh PV, Divyapriya G, Oturan N, Trellu C, Oturan MA (2019). Environmental applications of boron doped diamond electrode: 1. Applications in water and wastewater treatment. ChemElectrochem 6, 2124–2142.
| Environmental applications of boron doped diamond electrode: 1. Applications in water and wastewater treatmentCrossref | GoogleScholarGoogle Scholar |
Oturan MA (2000). An ecologically effective water treatment technique using electrochemically generated hydroxyl radicals for in situ destruction of organic pollutants. Application to herbicide 2,4-D. Journal of Applied Electrochemistry 30, 477–482.
Oturan MA, Aaron J-J (2014). Advanced oxidation processes in water/wastewater treatment: principles and applications. A review. Critical Reviews in Environmental Science and Technology 44, 2577–2641.
| Advanced oxidation processes in water/wastewater treatment: principles and applications. A reviewCrossref | GoogleScholarGoogle Scholar |
Oturan N, Oturan MA (2018). Electro-Fenton process: background, new developments and applications. In ‘Electrochemical water treatment methods’. (Eds CA Martínez-Huitle, MA Rodrigo, O Scialdone) pp. 1–32. (Elsevier: Amsterdam)
Oturan MA, Peiroten J, Chartrin P, Acher AJ (2000). Complete destruction of p-nitrophenol in aqueous medium by electro-Fenton method. Environmental Science & Technology 34, 3474–3479.
| Complete destruction of p-nitrophenol in aqueous medium by electro-Fenton methodCrossref | GoogleScholarGoogle 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. Environmental Chemistry Letters 10, 165–170.
| Unprecedented total mineralization of atrazine and cyanuric acid by anodic oxidation and electro-Fenton with a boron-doped diamond anodeCrossref | GoogleScholarGoogle Scholar |
Özcan A, Şahin Y, Oturan MA (2013). Complete removal of the insecticide azinphos-methyl from water by the electro-Fenton method – A kinetic and mechanistic study. Water Research 47, 1470–1479.
| Complete removal of the insecticide azinphos-methyl from water by the electro-Fenton method – A kinetic and mechanistic studyCrossref | GoogleScholarGoogle Scholar | 23276423PubMed |
Panizza M, Cerisola G (2001). Removal of organic pollutants from industrial wastewater by electrogenerated Fenton’s reagent. Water Research 35, 3987–3992.
| Removal of organic pollutants from industrial wastewater by electrogenerated Fenton’s reagentCrossref | GoogleScholarGoogle Scholar | 12230183PubMed |
Panizza M, Cerisola G (2005). Application of diamond electrodes to electrochemical processes. Electrochimica Acta 51, 191–199.
| Application of diamond electrodes to electrochemical processesCrossref | GoogleScholarGoogle Scholar |
Panizza M, Cerisola G (2009). Direct and mediated anodic oxidation of organic pollutants. Chemical Reviews 109, 6541–6569.
| Direct and mediated anodic oxidation of organic pollutantsCrossref | GoogleScholarGoogle Scholar | 19658401PubMed |
Randazzo S, Scialdone O, Brillas E, Sirés I (2011). Comparative electrochemical treatments of two chlorinated aliphatic hydrocarbons. Time course of the main reaction by-products. Journal of Hazardous Materials 192, 1555–1564.
| Comparative electrochemical treatments of two chlorinated aliphatic hydrocarbons. Time course of the main reaction by-productsCrossref | GoogleScholarGoogle Scholar | 21783322PubMed |
Ren G, Zhou M, Su P, Yang W, Lu X, Zhang Y (2019). Simultaneous sulfadiazines degradation and disinfection from municipal secondary effluent by a flow-through electro-Fenton process with graphene-modified cathode. Journal of Hazardous Materials 368, 830–839.
| Simultaneous sulfadiazines degradation and disinfection from municipal secondary effluent by a flow-through electro-Fenton process with graphene-modified cathodeCrossref | GoogleScholarGoogle Scholar | 30743230PubMed |
Rodrigo MA, Cañizares P, Sánchez-Carretero A, Sáez C (2010). Use of conductive-diamond electrochemical oxidation for wastewater treatment. Catalysis Today 151, 173–177.
| Use of conductive-diamond electrochemical oxidation for wastewater treatmentCrossref | GoogleScholarGoogle Scholar |
Sirés I, Brillas E (2012). Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies: a review. Environment International 40, 212–229.
| Remediation of water pollution caused by pharmaceutical residues based on electrochemical separation and degradation technologies: a reviewCrossref | GoogleScholarGoogle Scholar | 21862133PubMed |
Sirés I, Garrido JA, Rodríguez RM, Brillas E, Oturan N, Oturan MA (2007). Catalytic behavior of the Fe3+/Fe2+ system in the electro-Fenton degradation of the antimicrobial chlorophene. Applied Catalysis B: Environmental 72, 382–394.
| Catalytic behavior of the Fe3+/Fe2+ system in the electro-Fenton degradation of the antimicrobial chloropheneCrossref | GoogleScholarGoogle Scholar |
Sirés I, Brillas E, Oturan MA, Rodrigo MA, Panizza M (2014). Electrochemical advanced oxidation processes: today and tomorrow. A review. Environmental Science and Pollution Research International 21, 8336–8367.
| Electrochemical advanced oxidation processes: today and tomorrow. A reviewCrossref | GoogleScholarGoogle Scholar | 24687788PubMed |
Sopaj F, Oturan N, Pinson J, Podvorica F, Oturan MA (2016). Effect of the anode materials on the efficiency of the electro-Fenton process for the mineralization of the antibiotic sulfamethazine. Applied Catalysis B: Environmental 199, 331–341.
| Effect of the anode materials on the efficiency of the electro-Fenton process for the mineralization of the antibiotic sulfamethazineCrossref | GoogleScholarGoogle Scholar |
Vergili I, Kaya Y, Gönder ZB, Boergers A, Tuerk J (2019). Occurence and prioritization of pharmaceutical active compounds in domestic / municipal wastewater treatment plants. Bulletin of Environmental Contamination and Toxicology 102, 252–258.
| Occurence and prioritization of pharmaceutical active compounds in domestic / municipal wastewater treatment plantsCrossref | GoogleScholarGoogle Scholar | 30666389PubMed |
Yang W, Zhou M, Oturan N, Lia Y, Oturan MA (2019). Electrocatalytic destruction of pharmaceutical imatinib by electro-Fenton process with graphene-based cathode. Electrochimica Acta 305, 285–294.
Zhang H, Fei C, Zhang D, Tang F (2007). Degradation of 4-nitrophenol in aqueous medium by electro-Fenton method. Journal of Hazardous Materials 145, 227–232.
| Degradation of 4-nitrophenol in aqueous medium by electro-Fenton methodCrossref | GoogleScholarGoogle Scholar | 17161909PubMed |