key: cord-0881649-rjwtg19i authors: Midassi, Sondos; Bedoui, Ahmed; Bensalah, Nasr title: Efficient degradation of chloroquine drug by electro-Fenton oxidation: Effects of operating conditions and degradation mechanism date: 2020-07-10 journal: Chemosphere DOI: 10.1016/j.chemosphere.2020.127558 sha: 81e91fe428026ecfa945c38d8f158785d6e5ccfd doc_id: 881649 cord_uid: rjwtg19i In this work, the degradation of chloroquine (CLQ), an antiviral and antimalarial drug, using electro-Fenton oxidation was investigated. Due to the importance of hydrogen peroxide (H(2)O(2)) generation during electro-Fenton oxidation, effects of pH, current density, molecular oxygen (O(2)) flow rate, and anode material on H(2)O(2) generation were evaluated. H(2)O(2) generation was enhanced by increasing the current density up to 60 mA/cm(2) and the O(2) flow rate up to 80 mL/min at pH 3.0 and using carbon felt cathode and boron-doped diamond (BDD) anode. Electro-Fenton-BDD oxidation achieved the total CLQ depletion and 92% total organic carbon (TOC) removal. Electro-Fenton-BDD oxidation was more effective than electro-Fenton-Pt and anodic oxidation using Pt and BDD anodes. The efficiency of CLQ depletion by electro-Fenton-BDD oxidation raises by increasing the current density and Fe(2+) dose; however it drops with the increase of pH and CLQ concentration. CLQ depletion follows a pseudo-first order kinetics in all the experiments. The identification of CLQ degradation intermediates by chromatography methods confirms the formation of 7-chloro-4-quinolinamine, oxamic, and oxalic acids. Quantitative amounts of chlorides, nitrates, and ammonium ions are released during electro-Fenton oxidation of CLQ. The high efficiency of electro-Fenton oxidation derives from the generation of hydroxyl radicals from the catalytic decomposition of H(2)O(2) by Fe(2+) in solution, and the electrogeneration of hydroxyl and sulfates radicals and other strong oxidants (persulfates) from the oxidation of the electrolyte at the surface BDD anode. Electro-Fenton oxidation has the potential to be an alternative method for treating wastewaters contaminated with CLQ and its derivatives. CLQ N4-(7-Chloro-4-quinolyl)-N1,N1-diethyl-1,4-pentanediamine Diphosphate (see 125 Table 1 ) was purchased from VWR (with purity ≥ 98%). 7-chloro-4-quinolinamine (4-126 Amino-7-chloroquinoline) (CQLA) was obtained from Sigma-Aldrich (see Table 1 ). Oxalic acid (OAA) (anhydrous, ≥ 98.0) and oxamic acid (OAMA) (anhydrous, ≥ 97.0) 128 were received from VWR (see Table 1 respectively. Fitting the data to pseudo-first order kinetics showed that the rate constant 424 k obs increased linearly with current density between 20 and 100 mA/cm 2 , then it became 425 almost unvaried with the increase of the current density (see inlet graph in Figure 5 ). The specific electric charge consumption calculated from the following formula: Table 2 . Estimated specific electric charge consumption during electro-Fenton oxidation of 125 mg/L CLQ aqueous solutions using carbon felt cathode and BDD anode at different current densities (same experimental conditions than Figure 2 ). Time required for complete CLQ depletion -Chloroquine, an antiviral drug, has the potential to be persistent pollutant in water -Effective H 2 O 2 generation was obtained by pairing carbon felt cathode and BDD anode -Electro-Fenton-BDD depleted chloroquine from water independently of operating conditions -Chloroquine degradation leads to the formation of aromatic intermediates and carboxylic acids -Electro-Fenton achieved the release of Clions and conversion of organic nitrogen to NO 3 and NH 4 + Advanced oxidation processes for 596 in-situ production of hydrogen peroxide/hydroxyl radical for textile wastewater 597 treatment: A review Advanced oxidation processes for 599 in-situ production of hydrogen peroxide/hydroxyl radical for textile wastewater 600 treatment: A review A review on Fenton and improvements to 602 the Fenton process for wastewater treatment A review on Fenton and improvements to 605 the Fenton process for wastewater treatment Treatment of persistent 608 organic pollutants in wastewater using hydrodynamic cavitation in synergy with 609 advanced oxidation process Treatment of Photographic Processing Wastewater Efficient degradation of tannic acid in water 615 by UV/H2O2 process The contribution of mediated oxidation 618 mechanisms in the electrolytic degradation of cyanuric acid using diamond anodes Wastewater treatment by means of advanced 621 oxidation processes at basic pH conditions: A review Review of iron-free Fenton-like systems for activating 624 H2O2 in advanced oxidation processes Anodic oxidation, electro-Fenton and 627 photoelectro-Fenton degradation of cyanazine using a boron-doped diamond 628 anode and an oxygen-diffusion cathode Applied Catalysis B : Environmental 631 Decontamination of wastewaters containing synthetic organic dyes by 632 electrochemical methods : A general review Electro-fenton and photoelectro-fenton degradation of sulfanilic 678 acid using a boron-doped diamond anode and an air diffusion cathode The synergic persulfate-sodium dodecyl sulfate effect during the electro-682 oxidation of caffeine using active and non-active anodes Patterns of chloroquine use and 685 resistance in sub-Saharan Africa: A systematic review of household survey and 686 molecular data Pharmacokinetics of hydroxychloroquine and chloroquine during 688 treatment of rheumatic diseases Wastewater treatment by means of 691 advanced oxidation processes based on cavitation -A review Breakthrough: Chloroquine phosphate has shown 694 apparent efficacy in treatment of COVID-19 associated pneumonia in clinical 695 studies Enhancement 697 of oxygen reduction on a newly fabricated cathode and its application in the electro-698 Fenton process Mineralization of the recalcitrant oxalic and oxamic 700 acids by electrochemical advanced oxidation processes using a boron-doped 701 diamond anode Environmental Implications 703 of Hydroxyl Radicals (•OH) Partial degradation of 705 levofloxacin for biodegradability improvement by electro-Fenton process using an 706 activated carbon fiber felt cathode Indirect Electrochemical Oxidation Using Hydroxyl Radical Electrochemical Water and Wastewater 710 Treatment Degradation of the fluoroquinolone enrofloxacin by electrochemical 713 advanced oxidation processes based on hydrogen peroxide electrogeneration anoxic/oxic-dynamic membrane bioreactor (A/O-DMBR) Electrochemical oxidation of hydroquinone, resorcinol, and catechol on boron-760 doped diamond anodes Photochemical stability of biologically 762 active compounds. IV. 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