Electro-Fenton degradation of the antibiotic sulfanilamide with Pt/carbon-felt and BDD/carbon-felt cells. Kinetics,reaction intermediates,and toxicity assessment

The degradation of 230 mL of a 0.6-mM sulfanilamide solution in 0.05 M Na₂SO₄ of pH 3.0 has been studied by electro-Fenton process. The electrolytic cell contained either a Pt or boron-doped diamond (BDD) anode and a carbon-felt cathode. Under these conditions, organics are oxidized by hydroxyl radicals formed at the anode surface from water oxidation and in the bulk from Fenton’s reaction between initially added (and then electrochemically regenerated) Fe²⁺ and cathodically generated H₂O₂. From the decay of sulfanilamide concentration determined by reversed-phase liquid chromatography, an optimum Fe²⁺ concentration of 0.20 mM in both cells was found. The drug disappeared more rapidly using BDD than Pt, and, in both cases, it was more quickly removed with raising applied current. Almost total mineralization was achieved using the BDD/carbon-felt cell, whereas the alternative use of Pt anode led to a slightly lower mineralization degree. In both cells, the degradation rate was accelerated at higher current but with the concomitant fall of mineralization current efficiency due to the greater increase in rate of the parasitic reactions of hydroxyl radicals. Reversed-phase liquid chromatography allowed the identification of catechol, resorcinol, hydroquinone, p-benzoquinone, and 1,2,4-trihydroxybenzene as aromatic intermediates, whereas ion exclusion chromatography revealed the formation of malic, maleic, fumaric, acetic, oxalic, formic, and oxamic acids. NH₄ ⁺, NO₃ ^?, and SO₄ ^2? ions were released during the electro-Fenton process. A plausible reaction sequence for sulfanilamide mineralization involving all detected intermediates has been proposed. The toxicity of the solution was assessed from the Vibrio fischeri bacteria luminescence inhibition. Although it acquired its maximum value at short electrolysis time, the solution was completely detoxified at the end of the electro-Fenton treatment, regardless of the anode used.     

Degradation of Acid Orange 7 by electrochemically generated (*)OH radicals in acidic aqueous medium using a boron-doped diamond or platinum anode: a mechanistic study

A comparative study of the degradation of Acid Orange 7 (AO 7) aqueous solutions in acidic medium of pH 3.0 by electro-Fenton process using Pt or boron-doped diamond (BDD) anode was reported. The oxidative degradation of AO 7 by electrochemically generated hydroxyl radicals follows a pseudo-first order kinetic with a similar rate constant with BDD or Pt anode. The absolute rate constant of the AO 7 hydroxylation reaction was determined as (1.10+/-0.04)x10(10)M(-1)s(-1) by using the competition kinetic method. The comparative study of TOC measurements during electro-Fenton treatment showed a higher mineralization rate with BDD than Pt anode at the first hours of electrolysis because of the higher oxidizing power of this anode. The electro-Fenton degradation of AO 7 was followed by monitoring the formation and evolution of aromatic intermediates which are oxidized to aliphatic carboxylic acids before mineralization (transformation to CO(2) and inorganic ions, i.e. sulphate, nitrate and ammonium). The follow-up of the solution toxicity evolution shows the formation of intermediates more toxic than AO 7 and the connection between toxicity and aromaticity. A mineralization reaction pathway of AO 7 by electro-Fenton degradation involving all the intermediates identified was proposed.     

Evaluation of microbial contamination and distribution of sulphate-reducing bacteria in dental units

Although bacterial contamination is widely researched in dental unit water systems, we have been unable to find any published reports to date about the presence and distribution of sulphate-reducing bacteria (SRB) in dental unit waterlines (DUWLs). The aim of this study was to evaluate microbial contamination and to determine the presence and distribution of SRB in DUWLs. One hundred twenty-three water samples were collected from the air–water syringes, high-speed drills and water sources from 41 dental units in Istanbul, Turkey. The counts of aerobic heterotrophic bacteria and SRB were investigated in the water samples. In addition, the presence of free-living amoebae (FLA) was examined. In this work, we evaluated microbial contamination and reported for the first time the distribution of SRB in DUWLs. We determined that only ten out of 123 water samples were able to meet the American Dental Association’s limit (≤200 CFU ml^− 1). SRB were observed in 102 out of 123 samples (82.9%). In addition, SRB were detected in all of the air–water syringes and high-speed drills. FLA were established in 103 out of 123 samples (83.7%).     

Removal of organochlorine pesticides from lindane production wastes by electrochemical oxidation

This study is focused on the effective removal of recalcitrant pollutants hexaclorocyclohexanes (HCHs, isomers α, β, γ, and δ) and chlorobenzenes (CBs) present in a real groundwater coming from a landfill of an old lindane factory. Groundwater is characterized by a total organic carbon (TOC) content of 9 mg L^?1, pH₀?=?7, conductivity?=?3.7 mS cm^?1, high salt concentration (SO₄^2?, HCO₃^?, Cl^?), and ferrous iron in solution. The experiments were performed using a BDD anode and a carbon felt (CF) cathode at the natural groundwater pH and without addition of supporting electrolyte. The complete depletion of the four HCH isomers and a mineralization degree of 90% were reached at 4-h electrolysis with a current intensity of 400 mA, the residual TOC (0.8 mg L^?1) corresponding mainly to formic acid. A parallel series reaction pathway was proposed: HCHs and CBs are transformed into chlorinated and hydroxylated intermediates that are rapidly oxidized to non-toxic carboxylic acids and/or mineralized, leading to a rapid decrease in solution pH.     

Removal of textile dyes from water by the electro-Fenton process

An environmentally friendly electrochemical treatment, electro-Fenton process, was applied to the depollution of a synthetic dismissal composed of three dyes, yellow drimaren, congo red and methylene blue, frequently used in textile and dyehouses. Here, we show that those dyes and their mixture are quickly degraded under current controlled electrolysis conditions, leading to an almost complete mineralization. The results show the efficiency of electro-Fenton process to quickly degrade aqueous effluents polluted by synthetic organic dyes.     

Degradation of diuron by the electro-Fenton process

The degradation of the herbicide diuron has been undertaken by electrochemical advanced oxidation in aqueous solution. This process generates catalytically hydroxyl radicals that are strong oxidizing reagents for the oxidation of organic substances. Hydroxyl radicals degrade diuron in less than 10 min. Kinetic results evidence a pseudo-first-order degradation, with a rate constant of reaction between diuron and hydroxyl radicals of 4.8x10⁹ M^–1 s^–1. Several degradation products were identified by chromatography-mass spectrometry (LC-MS). The mineralization degree of a 1.7x10^–4 M diuron solution reached 93% at 1,000 coulombs.     

Removal of boron by electrocoagulation

Boron compounds are used in many manufacturing products and may be introduced into the environment in the form of hazardous materials. Here the feasibility of removal of boron from aqueous solutions by electrocoagulation was investigated. The process was examined under various factors in order to assess optimal operating conditions. The results showed that electrocoagulation for boron removal depends on current density, initial concentration and time. Under a current density of 30 mA/cm² the percentage of boron removal from aqueous solutions is in the range of 92–96%.     

Removal of organophosphorus pesticides from water by electrogenerated Fenton's reagent

Aqueous solutions of organophosphorus pesticides were completely mineralized via in-situ generated hydroxyl radicals (HO^·) by the Electro-Fenton process. Formation of Fenton's reagent (H₂O₂, Fe²⁺) was carried out by simultaneous reduction of O₂ and Fe³⁺ on carbon cathode in acidic medium. The electrochemistry combined with Fenton's reagent provides an excellent way to continuously produce the hydroxyl radical, a powerful oxidant. We demonstrate the efficiency of the Electro-Fenton process to degrade three organophosphorus insecticides: malathion, parathion ethyl and tetra-ethyl-pyrophosphate (TEPP). Degradation kinetics and removals of chemical oxygen demand (COD) have been investigated. Here we show that the mineralization efficiency was over 80% for three organophosphorus pesticides.     

Unprecedented total mineralization of atrazine and cyanuric acid by anodic oxidation and electro-Fenton with a boron-doped diamond anode

This article reports the complete mineralization of atrazine. Atrazine has been the most widely used s-triazine herbicide. Atrazine occurs in natural waters and presents a potential danger for public health because atrazine is considered as an endocrine disruptor. The use of chemical, photochemical and photocatalytic advanced oxidation processes (AOPs) to decontaminate waters containing atrazine only allowed its conversion into the cyanuric acid as ultimate end products, since it cannot be completely degraded by hydroxyl radicals (^•OH) produced by these techniques. The same behavior was previously reported for anodic oxidation and electro-Fenton with Pt anode, although better performances were found using boron-doped diamond (BDD) anode but without explaining the role of generated ^•OH. Here, the oxidative action of these radicals in such electrochemical AOPs has been clarified by studying the mineralization process and decay kinetics of atrazine and cyanuric acid in separated solutions by anodic oxidation with BDD and electro-Fenton with Pt or BDD anode using an undivided cell with a carbon-felt cathode under galvanostatic conditions. Results showed that electro-Fenton with BDD anode was the more powerful treatment to degrade both compounds. Almost total mineralization, 97% total organic carbon (COT) removal, of atrazine was only feasible by this method with a faster removal of its oxidation intermediates by ^•OH formed at the BDD surface than that formed in the bulk from Fenton reaction, although the latter process caused a more rapid decay of the herbicide. Cyanuric acid was much slowly mineralized mainly with ^•OH produced at the BDD surface, and it was not degraded by electro-Fenton with Pt anode. These results highlight that electrochemical advanced oxidation processes (EAOPs) using a BDD anode are more powerful than the classical electro-Fenton process with Pt or PbO₂ anodes.