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1.
Environ Res ; 204(Pt A): 111898, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-34450155

RESUMO

This study investigated the degradation of the antineoplastic agent 5-fluorouracil (5-FU) widely applied to treat different cancers using different advanced oxidation processes such as electro-Fenton (EF), photocatalysis with TiO2, and H2O2-modified subcritical water oxidation. The treatment with the EF process was the most efficient compared to others. Interestingly, in the EF process, the oxidative degradation of 5-FU behaved differently depending on the anode used. At low currents (20 and 40 mA), Pt and DSA anodes performed better than BDD and Ti4O7 anodes. In contrast, at the higher current of 120 mA, the production of heterogeneous hydroxyl radicals (M(•OH)) became important and contributed significantly to the oxidation of 5-FU in addition to homogeneous •OH generated in the bulk solution. These latter have high O2-evolution overpotential leading to the high amount of physisorbed M(•OH) compared to Pt and DSA. The oxidative degradation of 5-FU was then performed by titanium dioxide-based photocatalytic oxidation and subcritical water oxidation processes, both of which showed a lower degradation efficiency and failed to achieve complete mineralization. Finally, a comparison was performed in laboratory-scale, taking into account the following performance indicators: the degradation efficiency, the mineralization power, the cost of equipment and reagents, and the energy required for the treatment of 5-FU.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Boro , Fluoruracila , Peróxido de Hidrogênio , Oxirredução , Água
2.
Environ Res ; 204(Pt D): 112353, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-34774509

RESUMO

This study aims to compare the efficiency of anodic oxidation with electrogenerated H2O2 (AO-H2O2), electro-Fenton (EF), and their association with UV irradiation (photo anodic oxidation (PAO), and photo electro-Fenton (PEF) for the removal of Direct Red 23 from wastewater using a BDD/carbon felt cell in chloride and sulfate medium and in their combination. The effect of the supporting electrolyte was investigated in AO-H2O2 and EF processes. High discoloration efficiency was obtained in chloride media while a higher mineralization rate was achieved in sulfate media. The EF process reached higher total organic carbon (TOC) removal efficiency than AO-H2O2. 90% TOC removal rate was achieved by the EF against 82% by AO-H2O2 in sulfate media. The influence of using the mixt supporting electrolyte formed of 75% Na2SO4 + 25% NaCl was found to have beneficial effect on TOC removal, achieving 89% and 97% by AO-H2O2 and EF, respectively. High currents led to higher mineralization rates while low currents yielded to a higher mineralization current efficiency (MCE%) and lower energy consumption (EC). UV irradiation enhanced process efficiency. Mineralization efficiency followed the sequence: AO-H2O2 < PAO < EF < PEF. The PEF process was able to remove TOC completely at 5 mA cm-2 current density and 6 h of electrolysis with a MCE% value of 16.57% and EC value of 1.29 kWh g-1 TOC removed.


Assuntos
Sulfatos , Poluentes Químicos da Água , Anilidas , Compostos Azo , Cloretos , Peróxido de Hidrogênio , Oxirredução , Poluentes Químicos da Água/análise
3.
Luminescence ; 34(5): 489-499, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-30972923

RESUMO

To develop conducting organic polymers (COPs) as luminescent sensors for determination of toxic heavy metals, a new benzene sulfonic acid-doped polypyrrole (PPy-BSA) thin film was electrochemically prepared by cyclic voltammetry (CV) on flexible indium tin oxide (ITO) electrode in aqueous solution. PPy-BSA film was characterized by FTIR spectrometry, X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). The optical properties of PPy-BSA were investigated by ultraviolet (UV)-visible absorption and fluorescence spectrometry in dimethylsulfoxide (DMSO) diluted solutions. PPy-BSA fluorescence spectra were strongly quenched upon increasing copper(II) ion (Cu2+ ) and lead(II) ion (Pb2+ ) concentrations in aqueous medium, and linear Stern-Volmer relationships were obtained, which indicated the existence of a main dynamic fluorescence quenching mechanism. BSA-PPy sensor showed a high sensitivity for detection of both metallic ions, Cu2+ and Pb2+ , with very low limit of detection values of 3.1 and 18.0 nM, respectively. The proposed quenching-fluorimetric sensor might be applied to the determination of traces of toxic heavy metallic ions in water samples.


Assuntos
Benzeno/química , Cobre/análise , Fluorometria/métodos , Chumbo/análise , Polímeros/química , Pirróis/química , Ácidos Sulfônicos/química , Poluentes Químicos da Água/análise , Fluorometria/instrumentação
4.
Luminescence ; 34(5): 465-471, 2019 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-30784165

RESUMO

Diflubenzuron (DFB) and fenuron (FEN) are benzoylurea and phenylurea pesticides, widely used in Senegal, that do not exhibit any natural fluorescence, but can be determined by means of photoinduced fluorescence (PIF) methods. Photodegradation of DFB and FEN yielded a number of fluorescent and non-fluorescent photoproducts. For both pesticides, at least 10 photoproducts were detected and identified by gas chromatography-mass spectrometry (GC/MS). To identify the formed fluorescent DFB and FEN photoproducts, their fluorescence spectra were compared with those of standard compounds, including phenol and p-hydroxyaniline.


Assuntos
Diflubenzuron/química , Praguicidas/química , Compostos de Fenilureia/química , Fluorescência , Cromatografia Gasosa-Espectrometria de Massas , Fotólise , Raios Ultravioleta
5.
Environ Sci Technol ; 52(13): 7450-7457, 2018 07 03.
Artigo em Inglês | MEDLINE | ID: mdl-29856620

RESUMO

An electro-Fenton (EF) based technology using activated carbon (AC) fiber as cathode and BDD as anode has been investigated for both regeneration of AC and mineralization of organic pollutants. The large specific surface area and low intraparticle diffusion resistance of AC tissue resulted in high maximum adsorption capacity of phenol (PH) (3.7 mmol g-1) and fast adsorption kinetics. Spent AC tissue was subsequently used as the cathode during the EF process. After 6 h of treatment at 300 mA, 70% of PH was removed from the AC surface. The effectiveness of the process is ascribed to (i) direct oxidation of adsorbed PH by generated hydroxyl radicals, (ii) continuous shift of adsorption equilibrium due to oxidation of organic compounds in the bulk, and (iii) local pH change leading to electrostatic repulsive interactions. Moreover, 91% of PH removed from AC was completely mineralized, thus avoiding adsorption of degradation byproducts and accumulation of toxic compounds such as benzoquinone. Morphological and chemical characteristics of AC were not affected due to the effect of cathodic polarization protection. AC tissue was successfully reused during 10 cycles of adsorption/regeneration with regeneration efficiency ranging from 65 to 78%, in accordance with the amount of PH removed from the AC surface.


Assuntos
Fibra de Carbono , Poluentes Químicos da Água , Carbono , Carvão Vegetal , Eletrodos , Peróxido de Hidrogênio , Ferro , Oxirredução
6.
Environ Sci Technol ; 49(20): 12187-96, 2015 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-26378656

RESUMO

In recent years, electrochemical advanced oxidation processes have been shown to be an effective alternative for the removal of refractory organic compounds from water. This study is focused on the effective removal of recalcitrant organic matter (micropollutants, humic substances, etc.) present in municipal solid waste landfill leachates. A mixture of eight landfill leachates has been studied by the electro-Fenton process using a Pt or boron-doped diamond (BDD) anode and a carbon felt cathode or by the anodic oxidation process with a BDD anode. These processes exhibit great oxidation ability due to the in situ production of hydroxyl radicals ((•)OH), a highly powerful oxidizing species. Both electrochemical processes were shown to be efficient in the removal of dissolved total organic carbon (TOC) from landfill leachates. Regarding the electro-Fenton process, the replacement of the classical anode Pt by the anode BDD allows better performance in terms of dissolved TOC removal. The occurrence and removal yield of 19 polycyclic aromatic hydrocarbons, 15 volatile organic compounds, 7 alkylphenols, 7 polychlorobiphenyls, 5 organochlorine pesticides, and 2 polybrominated diphenyl ethers in landfill leachate were also investigated. Both electrochemical processes allow one to reach a quasicomplete removal (about 98%) of these organic micropollutants.


Assuntos
Eletroquímica/métodos , Compostos Orgânicos/isolamento & purificação , Poluentes Químicos da Água/isolamento & purificação , Carbono/isolamento & purificação , Eletricidade , Eletrodos , Filtração , Peróxido de Hidrogênio/química , Ferro/química , Oxirredução
7.
J Environ Manage ; 153: 40-7, 2015 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-25646675

RESUMO

In order to improve the efficiency of soil washing treatment of hydrocarbon contaminated soils, an innovative combination of this soil treatment technique with an electrochemical advanced oxidation process (i.e. electro-Fenton (EF)) has been proposed. An ex situ soil column washing experiment was performed on a genuinely diesel-contaminated soil. The washing solution was enriched with surfactant Tween 80 at different concentrations, higher than the critical micellar concentration (CMC). The impact of soil washing was evaluated on the hydrocarbons concentration in the leachates collected at the bottom of the soil columns. These eluates were then studied for their degradation potential by EF treatment. Results showed that a concentration of 5% of Tween 80 was required to enhance hydrocarbons extraction from the soil. Even with this Tween 80 concentration, the efficiency of the treatment remained very low (only 1% after 24 h of washing). Electrochemical treatments performed thereafter with EF on the collected eluates revealed that the quasi-complete mineralization (>99.5%) of the hydrocarbons was achieved within 32 h according to a linear kinetic trend. Toxicity was higher than in the initial solution and reached 95% of inhibition of Vibrio fischeri bacteria measured by Microtox method, demonstrating the presence of remaining toxic compounds even after the complete degradation. Finally, the biodegradability (BOD5/COD ratio) reached a maximum of 20% after 20 h of EF treatment, which is not enough to implement a combined treatment with a biological treatment process.


Assuntos
Técnicas Eletroquímicas/métodos , Recuperação e Remediação Ambiental/métodos , Poluição por Petróleo , Polissorbatos/química , Poluentes do Solo/química , Tensoativos/química , Biodegradação Ambiental , Solo/química
8.
Chemosphere ; 341: 140129, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37690550

RESUMO

The rapid and efficient mineralization of the chemotherapeutic drug busulfan (BSF) as the target pollutant has been investigated for the first time by three different heterogeneous EF systems that were constructed to ensure the continuous electro-generation of H2O2 and •OH consisting of: i) a multifunctional carbon felt (CF) based cathode composed of reduced graphene oxide (rGO), iron oxide nanoparticles and carbon black (CB) (rGO-Fe3O4/CB@CF), ii) rGO modified cathode (rGO/CB@CF) and rGO supported Fe3O4 (rGO-Fe3O4) catalyst and iii) rGO modified cathode (rGO/CB@CF) and multi walled carbon nanotube supported Fe3O4 (MWCNT-Fe3O4) catalyst. The effects of main variables, including the catalyst amount, applied current and initial pH were investigated. Based on the results, H2O2 was produced by oxygen reduction reaction (ORR) on the liquid-solid interface of both fabricated cathodes. •OH was generated by the reaction of H2O2 with the active site of ≡FeII on the surface of the multifunctional cathode and heterogeneous EF catalysts. Utilizing carbon materials with high conductivity, the redox cycling between ≡FeII and ≡FeIII was effectively facilitated and therefore promoted the performance of the process. The results demonstrated almost complete mineralization of BSF through the heterogeneous systems over a wide applicable pH range. According to the reusability and stability tests, multifunctional cathode exhibited outstanding performance after five consecutive cycles which is promising for the efficient mineralization of refractory organic pollutants. Moreover, intermediates products of BSF oxidation were identified and a plausible oxidation pathway was proposed. Therefore, this study demonstrates efficient and stable cathodes and catalysts for the efficient treatment of an anticancer active substance.


Assuntos
Poluentes Ambientais , Nanocompostos , Bussulfano , Compostos Férricos , Peróxido de Hidrogênio , Condutividade Elétrica , Fuligem , Compostos Ferrosos
9.
Environ Sci Technol ; 46(7): 4074-82, 2012 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-22332959

RESUMO

The electro-Fenton treatment of sulfachloropyridazine (SCP), a model for sulfonamide antibiotics that are widespread in waters, was performed using cells with a carbon-felt cathode and Pt or boron-doped diamond (BDD) anode, aiming to present an integral assessment of the kinetics, electrodegradation byproducts, and toxicity evolution. H(2)O(2) electrogeneration in the presence of Fe(2+) yielded (•)OH in the solution bulk, which acted concomitantly with (•)OH adsorbed at the anode (BDD((•)OH)) to promote the oxidative degradation of SCP (k(abs,SCP) = (1.58 ± 0.02) × 10(9) M(-1) s(-1)) and its byproducts. A detailed scheme for the complete mineralization was elucidated. On the basis of the action of (•)OH onto four different SCP sites, the pathways leading to total decontamination includes fifteen cyclic byproducts identified by HPLC and GC-MS, five aliphatic carboxylic acids, and a mixture of Cl(-), SO(4)(2-), NH(4)(+), and NO(3)(-) that accounted for 90-100% of initial Cl, S, and N. The time course of byproducts was satisfactorily correlated with the toxicity profiles determined from inhibition of Vibrio fischeri luminescence. 3-Amino-6-chloropyridazine and p-benzoquinone were responsible for the increased toxicity during the first stages. Independent electrolyses revealed that their toxicity trends were close to those of SCP. The formation of the carboxylic acids involved a sharp toxicity decrease, thus ensuring overall detoxification.


Assuntos
Antibacterianos/química , Antibacterianos/toxicidade , Técnicas Eletroquímicas/métodos , Sulfacloropiridazina/química , Sulfacloropiridazina/toxicidade , Aliivibrio fischeri/efeitos dos fármacos , Aliivibrio fischeri/metabolismo , Carbono/análise , Eletricidade , Eletrodos , Peróxido de Hidrogênio/química , Ferro/química , Cinética , Luminescência , Minerais/química , Compostos Orgânicos/análise , Oxirredução/efeitos dos fármacos , Soluções , Fatores de Tempo
10.
J Hazard Mater ; 437: 129326, 2022 09 05.
Artigo em Inglês | MEDLINE | ID: mdl-35714542

RESUMO

This study aimed at understanding the influence of the generation of oxidants in a heterogeneous way at boron-doped diamond (BDD) anode (anodic oxidation (AO)) or homogeneously in the bulk (electro-Fenton (EF)) during treatment of a textile industry wastewater. Both processes achieved high TOC removal. A yield of 95 % was obtained by combining EF with BDD anode during 6 h of treatment. The EF process was found to be faster and more efficient for discoloration of the effluent, whereas AO was more effective to limit the formation of degradation by-products in the bulk. An advantage of AO was to treat this alkaline effluent without any pH adjustment. Operating these processes under current limitation allowed optimizing energy consumption in both cases. However, using BDD anode led to the formation of very high concentration of ClO3-/ClO4- from Cl- oxidation (even at low current density), which appears as a key challenge for treatment of such effluent by AO. By comparison, EF with Pt anode strongly reduced the formation of ClO3-/ClO4-. Operating EF at low current density even maintained these concentrations below 0.5 % of the initial Cl- concentration. A trade-off should be considered between TOC removal and formation of toxic chlorinated by-products.


Assuntos
Águas Residuárias , Poluentes Químicos da Água , Boro , Diamante , Eletrodos , Peróxido de Hidrogênio , Oxirredução , Indústria Têxtil
11.
Sci Total Environ ; 791: 148107, 2021 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-34118668

RESUMO

Low yields of H2O2 and a narrow range of appropriate pH values have been two major drawbacks for electro-Fenton (EF) process. Herein, metal-free electrochemical advanced oxidation processes (EAOPs) were developed with nitrogen and sulfur co-doped electrochemically exfoliated graphene (N, S-EEGr) electrocatalysts, which was confirmed as an outstanding bifunctional catalyst for synchronous generation and activation of H2O2 via (2 + 1) e- consecutive reduction reactions. Specifically, two elements (N, S) in metal-free N, S-EEGr-CF cathode synergize to promote the formation of H2O2 followed by its activation. With N, S-EEGr-CF cathode, phenol of initial 50 mg L-1 could be effectively removed within pH 3-11 and 6.25 mA cm-2, and 100% removal efficiency could be achieved within 15-min even at neutral pH. The pseudo-first-order rate constant for phenol removal in metal-free EAOPs with N,S-EEGr-CF at neutral pH was 10 times higher than that with EF process. Detection of active species, coupled with decay kinetics with specific trapping agents, confirmed that OH was the dominant oxidizing species promoting removal efficiencies of organics (phenol, antibiotics and dyes) at pH 3 and pH 7. In the actual wastewater treatment, the synergistic effect of bifunctional catalyst would also be used for improving the degradation efficiency of organics. Thus, the metal-free EAOPs with N,S-EEGr-CF cathode may serve as an alternative in wastewater treatment with a broadened range of solution pH values and avoiding Fe2+ (catalyst) addition.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Eletrodos , Peróxido de Hidrogênio , Radical Hidroxila , Oxirredução , Poluentes Químicos da Água/análise
12.
Environ Sci Pollut Res Int ; 28(39): 55029-55040, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34128161

RESUMO

A simple, sensitive, and rapid spectrofluorimetric method was developed for the determination of the ß-blocker pindolol. The native fluorescence of pindolol was measured in different organic solvents and in cyclodextrin aqueous media. The highest fluorescence signal was obtained in 2-propanol at λem = 303 nm with λex = 260 nm. Analytical figures of merit for the spectrofluorimetric determination of pindolol were satisfactory, with wide linear dynamic range (LDR) values of two orders of magnitude, and rather low limit of detection (LOD) values between 0.2 and 8.7 ng/mL. Moreover, the addition of cyclodextrins (HP-ß-CD and ß-CD) in aqueous media enhanced the fluorescence of pindolol. In addition, the inclusion complexes of pindolol with cyclodextrins were investigated and the stability constants of complexes were calculated by means of the method of nonlinear regression (NLR). The method was successfully applied to the analysis of tap water and natural water samples, spiked with pindolol.


Assuntos
Ciclodextrinas , Pindolol , Espectrometria de Fluorescência
13.
J Hazard Mater ; 404(Pt A): 124137, 2021 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-33049627

RESUMO

A lot of soil (particularly, former industrial and military sites) has been contaminated by various highly toxic contaminants such as petroleum hydrocarbons, polycyclic aromatic hydrocarbons (PAHs), polychlorobiphenyls (PCBs) or chlorinated solvents. Soil remediation is now required for their promotion into new industrial or real estate activities. Therefore, the soil washing (SW) process enhanced by the use of extracting agents (EAs) such as surfactants or cyclodextrins (CDs) has been developed for the removal of hydrophobic organic compounds (HOCs) from contaminated soils. The use of extracting agents allows improving the transfer of HOCs from the soil-sorbed fraction to the washing solution. However, using large amount of extracting agents is also a critical drawback for cost-effectiveness of the SW process. The aim of this review is to examine how extracting agents might be recovered from SW solutions for reuse. Various separation processes are able to recover large amounts of extracting agents according to the physicochemical characteristics of target pollutants and extracting agents. However, an additional treatment step is required for the degradation of recovered pollutants. SW solutions may also undergo degradation processes such as advanced oxidation processes (AOPs) with in situ production of oxidants. Partial recovery of extracting agents can be achieved according to operating conditions and reaction kinetics between organic compounds and oxidant species. The suitability of each process is discussed according to the various physicochemical characteristics of SW solutions. A particular attention is paid to the anodic oxidation process, which allows either a selective degradation of the target pollutants or a complete removal of the organic load depending on the operating conditions.

14.
J Phys Chem A ; 114(39): 10605-11, 2010 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-20828190

RESUMO

The oxidative degradation of insecticide metomyl as active ingredient and of its commercial formulation Lanate 20 L by an electro-Fenton process using a carbon felt cathode and iron ions as catalyst was compared with different transition metal ions such as, cobalt, silver, and copper as catalyst to produce hydroxyl radicals. The effect of catalyst nature and concentration on the degradation kinetics and COD removal was investigated and optimized. For all metal ions under study as catalyst, there is an optimal concentration value for degradation kinetics and solution COD removal efficiency. Fe(III) was confirmed to be the most efficient catalyst among the metals ions tested. The metomyl oxidative degradation was found to obey apparent first-order reaction kinetics, and the absolute rate constant of the oxidation between metomyl and hydroxyl radicals at pH 3.0 was obtained by competitive kinetics method, being 5.42 × 10(9) L mol(-1) s(-1).

15.
Artigo em Inglês | MEDLINE | ID: mdl-20390909

RESUMO

An experimental parametric study was carried out to investigate the effects of [H(2)O(2)], [Fe(3 +)] and [H(2)O(2)]/[Fe(3 +)] ratio on the photo-Fenton degradation of a azo dye Basic Blue 41 (BB41) in aqueous solution. This method consists of coupling between Fenton's reagent and UV irradiation in order to catalyze the in situ generation of hydroxyl radicals, a powerful oxidizing agent which leads to degradation of organic pollutants until total mineralization. The kinetics study of the reaction between BB41 and hydroxyl radicals showed that the degradation of BB41 follows the first-order kinetics. It was found that the concentration of H(2)O(2) and ferric iron as well as their ratio [H(2)O(2)]/[Fe(3 +)] are key factors governing the removal of BB41 in aqueous medium and that the optimal ratio [H(2)O(2)]/[Fe(3 +)] is equal to 10 for 0.2 mM Fe(3 +) concentration. The initial BB41 concentration and the [H(2)O(2)]/[BB41] ratio are also found as significant operating parameters on the mineralization efficiency. The optimization of the operating conditions permitted to obtain a quasi-total mineralization of synthetic BB41 aqueous solutions. When these optimal conditions were applied to the real wastewater, 90% of TOC removal was obtained after 8 h of irradiation time.


Assuntos
Compostos Azo/química , Corantes/química , Compostos Férricos/química , Peróxido de Hidrogênio/química , Ferro/química , Cinética , Oxirredução , Fotoquímica
16.
Chemosphere ; 247: 125939, 2020 May.
Artigo em Inglês | MEDLINE | ID: mdl-32069720

RESUMO

The removal of the analgesic tramadol (TMD) from water was studied by electro-Fenton (EF) process using BDD anode. Hydroxyl radicals (OH) generated in this process are very strong oxidants and able to successfully oxidize TMD until its total mineralization in aqueous solution. The oxidative degradation of TMD was very rapid with complete disappearance of 0.1 mM (26.3 mg L-1) TMD in 10 min at 500 mA constant current electrolysis. The absolute (second order) rate constant for oxidation of TMD by OH was determined using competition kinetic method and found to be (5.59 ± 0.03) ✕ 109 M-1 s-1. The quasi-complete mineralization of the 0.1 mM TMD solution was obtained in 6 h electrolysis at 500 mA current. Several oxidation reaction intermediates were identified using GC-MS analysis. Oxalic, glyoxylic and fumaric acids were identified and their evolution during electrolysis was followed along treatment. Ammonium and nitrate ions, released during the treatment, were also considered. Based on these data and TOC removal results, a possible mineralization pathway was proposed.


Assuntos
Tramadol/química , Poluentes Químicos da Água/química , Analgésicos , Eletrodos , Eletrólise , Peróxido de Hidrogênio , Radical Hidroxila , Cinética , Oxidantes , Oxirredução , Platina
17.
Chemosphere ; 249: 126176, 2020 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-32087453

RESUMO

Sequential soil washing and electrochemical advanced oxidation processes (EAOPs) were applied for the remediation of synthetic soil contaminated with diesel. The surfactant Tween 80 was used to enhance the extraction of diesel from synthetic soil, and diesel extraction efficiency was improved with the increase of Tween 80 concentration. Under conditions of 180 min washing time, 10 g synthetic soil with 100 mL surfactant solution and two times of soil washing, about 75.2%, 80.0% and 87.9% of diesel was extracted from synthetic soil with 5.0, 7.5 and 10.0 g L-1 Tween 80. The degradation of diesel in soil washing effluent was carried out by two EAOPs, electro-oxidation (EO) and electro-Fenton (EF) using boron-doped diamond (BDD) anode and carbon felt cathode cell. After 360 min EO treatment, 72.7-83.0% of diesel was removed from the effluent after soil washing with 5.0-10.0 g L-1 Tween 80 while higher removal efficiencies (77.7-87.2%) were attained with EF process. Parallel factor analysis (PARAFAC) of excitation emission matrix (EEM) fluorescence spectroscopy was conducted to analysis the transformation of fluorescent components in diesel during the treatment by two EAOPs.


Assuntos
Recuperação e Remediação Ambiental/métodos , Gasolina/análise , Poluentes do Solo/química , Solo/química , Boro/química , Diamante/química , Técnicas Eletroquímicas/métodos , Eletrodos , Oxirredução , Polissorbatos/química , Tensoativos/química
18.
J Hazard Mater ; 393: 122513, 2020 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-32208334

RESUMO

The traditional electro-Fenton (EF) has been facing major challenges including narrow suitable range of pH and non-reusability of catalyst. To overcome these drawbacks we synthesized FeIIFeIII-layered double hydroxide modified carbon felt (FeIIFeIII LDH-CF) cathode via in situ solvo-thermal process. Chemical composition and electrochemical characterization of FeIIFeIII LDH-CF were tested and analyzed. The apparent rate constant of decay kinetics of ofloxacin (OFC) with FeIIFeIII LDH-CF (0.18 min-1) at pH 7 was more than 3 times higher than that of homogeneous EF (0.05 min-1) at pH 3 with 0.1 mM Fe2+ under same current density (9.37 mA cm-2). Also, a series of experiments including evolution of solution pH, iron leaching, OFC removal with trapping agent and quantitative detection of hydroxyl radicals (OH) were conducted, demonstrating the dominant role of OH generated by surface catalyst via ≡ FeII/FeIII on LDH cathode for degradation of organics as well contributing to high efficiency and good stability at neutral pH. Besides, formation and evolution of aromatic intermediates, carboxylic acids and inorganic ions (F-, NH4+ and NO3-) were identified by High-Performance Liquid chromatography, Gas Chromatography-Mass Spectrometry and ionic chromatography analyses. These findings allowed proposing a plausible degradation pathway of OFC by OH generated in the heterogeneous EF process.


Assuntos
Antibacterianos/química , Carbono/química , Hidróxidos/química , Ferro/química , Ofloxacino/química , Poluentes Químicos da Água/química , Eletrodos , Eletrólise , Concentração de Íons de Hidrogênio
19.
Chemosphere ; 253: 126659, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32278912

RESUMO

Combination of the electro-Fenton process with a post-biological treatment could represent a cost-effective solution for application of electrochemical advanced oxidation processes. The objective of this study was to assess this treatment strategy in the case of a complex pharmaceutical mixture. First, main operating parameters ([Fe2+] and current) of the electro-Fenton process were optimized. An optimal concentration of 0.2 mM of Fe2+ was obtained for mineralization of the pharmaceutical mixture. An optimal current of 400 mA was also obtained for degradation of caffeine and 5-fluorouracil in the mixture. However, mineralization of the effluent was continuously improved when increasing the current owing to the promotion of mineralization of organic compounds at the BDD anode. Besides, energy efficiency was decreased at prolonged treatment time because of mass transport limitation. Interestingly, it was observed a strong biodegradability enhancement of the solution after short treatment times (<3 h) at 500 and 1000 mA, which can be related to the degradation of parent compounds into more biodegradable by-products. The need for an acclimation time of the biomass to the pre-treated effluent was also emphasized, most probably because of the formation of some toxic by-products as observed during acute toxicity tests. Therefore, a biological post-treatment could represent a cost-effective solution for the removal of biodegradable residual organic compounds as well as for the removal of nitrogen released from mineralization of organic compounds under the form of NO3- and NH4+ during electro-Fenton pre-treatment.


Assuntos
Biodegradação Ambiental , Poluentes Químicos da Água/química , Purificação da Água/métodos , Eletrodos , Peróxido de Hidrogênio/química , Nitrogênio , Oxirredução
20.
J Phys Chem A ; 113(41): 10988-93, 2009 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-19764768

RESUMO

This study reports the kinetics of the degradation of several chlorophenols (CPs), such as monochlorophenols (2-chlorophenol and 4-chlorophenol), dichlorophenols (2,4-dichlorophenol and 2,6- dichlorophenol), trichlorophenols (2,3,5- trichlorophenol and 2,4,5-trichlorophenol), 2,3,5,6-tetrachlorophenol, and pentachlorophenol, by the electro-Fenton process using a carbon felt cathode and a Pt anode. The effect of number and the position of the chlorine atoms in the aromatic ring on the oxidative degradation rate was evaluated and discussed. The oxidation reaction of all the CPs with hydroxyl radicals evidenced a pseudo-first-order kinetics and the rate constant decreased with increasing the number of chlorine atoms. The absolute rate constant of second-order reaction kinetics between CPs and (*)OH was determined by the competition kinetics method in the range of (3.56-7.75) x 10(9) M(-1) s(-1) and follows the same sequence of the apparent rate constants. The mineralization of several CPs and of a mixture of all CPs under study was monitored by the total organic carbon (TOC) removal and the chlorine release during mineralization was followed by ion chromatography. Our results demonstrated that more chlorinated phenols are more difficult to mineralize; however for all the tested CPs, almost quantitative release of chloride ions was obtained after 6 h of treatment.

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