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1.
J Environ Manage ; 370: 122797, 2024 Oct 08.
Article in English | MEDLINE | ID: mdl-39383744

ABSTRACT

Glyphosate (GLY), a globally-used organophosphate herbicide, is frequently detected in various environmental matrices, including water, prompting significant attention due to its persistence and potential ecological impacts. In light of this environmental concern, innovative remediation strategies are warranted. This study utilized Serratia sp. AC-11 isolated from a tropical peatland as a biocatalyst in a microbial fuel cell (MFC) coupled with a homogeneous electron-Fenton (EF) process to degrade glyphosate in aqueous medium. After coupling the processes with a resistance of 100 Ω, an output voltage value of 0.64 V was obtained and maintained stable throughout the experiment. A bacterial biofilm of Serratia sp. AC-11 was formed on the carbon felt electrode, confirmed by attenuated total reflectance-Fourier transformed infrared (ATR-FTIR) and scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). In the anodic chamber, the GLY biodegradation rate was 100% after 48 h of experimentation, with aminomethylphosphonic acid (AMPA) remaining in the solution. In the cathodic chamber, the GLY degradation rate for the EF process was 69.5% after 48 h experimentation, with almost all of the AMPA degraded by the in situ generated hydroxyl radicals. In conclusion, the results demonstrated that Serratia sp. AC-11 not only catalyzed the biodegradation of glyphosate but also facilitated the generation of electrons for subsequent transfer to initiate the EF reaction to degrade glyphosate. This dual functionality emphasizes the unique capabilities of Serratia sp. AC-11, it as an electrogenic microorganism with application in innovative bioelectrochemical processes, and highlighting its role in sustainable strategies for environmental remediation.

2.
Chemosphere ; 363: 142825, 2024 Sep.
Article in English | MEDLINE | ID: mdl-38996982

ABSTRACT

Electrochemical oxidation (EO), electro-Fenton (EF), and photoelectro-Fenton (PEF) with a BDD anode have been comparatively assessed to remediate solutions of Red CL and/or Red WB azo dyes from real raw water. For the EO process in 50 mM Na2SO4 at pH 3.0, the main oxidant was the heterogeneous •OH generated at the anode, whereas in EF and PEF, the cathodic production of H2O2 and the addition of 0.50 mM Fe2+ catalyst additionally originated homogeneous •OH that enhanced the oxidation of organics. In PEF, the solution was illuminated with a 6 W UVA light. An almost total discoloration was always found operating with a 1:1 mixture of 200 mg L-1 of both dyes in 60 min, whose efficiency increased in the order of EO < EF < PEF. The HPLC analysis of the dye mixture treated by PEF disclosed that its degradation process agreed with its discoloration. A high 74% of COD was reduced due to the oxidative action of hydroxyl radicals and the photolysis of final Fe(III)-carboxylate species with UVA irradiation. The process was accompanied by an energy consumption of 0.76 kWh (g COD)-1, a value similar to the energy consumed by the applied UVA light.


Subject(s)
Azo Compounds , Boron , Coloring Agents , Diamond , Electrodes , Oxidation-Reduction , Water Pollutants, Chemical , Coloring Agents/chemistry , Water Pollutants, Chemical/chemistry , Boron/chemistry , Azo Compounds/chemistry , Diamond/chemistry , Hydrogen Peroxide/chemistry , Tanning , Electrochemical Techniques , Photolysis , Ultraviolet Rays , Waste Disposal, Fluid/methods , Iron/chemistry
3.
Chemosphere ; 361: 142515, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38830460

ABSTRACT

The catalytic performance of modified hydroxyapatite nanoparticles, Ca10-xFex-yWy(PO4)6(OH)2, was applied for the degradation of methylene blue (MB), fast green FCF (FG) and norfloxacin (NOR). XPS analysis pointed to the successful partial replacement of Ca by Fe. Under photo-electro-Fenton process, the catalyst Ca4FeII1·92W0·08FeIII4(PO4)6(OH)2 was combined with UVC radiation and electrogenerated H2O2 in a Printex L6 carbon-based gas diffusion electrode. The application of only 10 mA cm-2 resulted in 100% discoloration of MB and FG dyes in 50 min of treatment at pH 2.5, 7.0 and 9.0. The proposed treatment mechanism yielded maximum TOC removal of ∼80% and high mineralization current efficiency of ∼64%. Complete degradation of NOR was obtained in 40 min, and high mineralization of ∼86% was recorded after 240 min of treatment. Responses obtained from LC-ESI-MS/MS are in line with the theoretical Fukui indices and the ECOSAR data. The study enabled us to predict the main degradation route and the acute and chronic toxicity of the by-products formed during the contaminants degradation.


Subject(s)
Electrodes , Hydrogen Peroxide , Iron , Methylene Blue , Nanoparticles , Water Pollutants, Chemical , Catalysis , Hydrogen Peroxide/chemistry , Iron/chemistry , Methylene Blue/chemistry , Nanoparticles/chemistry , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Norfloxacin/chemistry , Durapatite/chemistry , Coloring Agents/chemistry , Photochemical Processes , Ultraviolet Rays
4.
Chemosphere ; 360: 142372, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38768783

ABSTRACT

The present study demonstrates, for the first time, the feasibility of a two-step process consisting of Electro-Fenton (EF) followed by microalgae to treat highly loaded real food processing wastewater along with resource recovery. In the first step, EF with a carbon felt cathode and Ti/RuO2-IrO2 anode was applied at different current densities (3.16 mA cm-2, 4.74 mA cm-2 and 6.32 mA cm-2) to decrease the amount of organic matter and turbidity and enhance biodegradability. In the second step, the EF effluents were submitted to microalgal treatment for 15 days using a mixed culture dominated by Scenedesmus sp., Chlorosarcinopsis sp., and Coelastrum sp. Results showed that current density impacted the amount of COD removed by EF, achieving the highest COD removal of 77.5% at 6.32 mA cm-2 with >95% and 74.3% of TSS and PO43- removal, respectively. With respect to microalgae, the highest COD removal of 85% was obtained by the culture in the EF effluent treated at 6.32 mA cm-2. Remarkably, not only 85% of the remaining organic matter was removed by microalgae, but also the totality of inorganic N and P compounds, as well as 65% of the Fe catalyst that was left after EF. The removal of inorganic species also demonstrates the high complementarity of both processes, since EF does not have the capacity to remove such compounds, while microalgae do not grow in the raw wastewater. Furthermore, a maximum of 0.8 g L-1 of biomass was produced after cultivation, with an accumulation of 32.2% of carbohydrates and 25.9% of lipids. The implementation of the two processes represents a promising sustainable approach for the management of industrial effluents, incorporating EF in a water and nutrient recycling system to produce biomass that could be valorized into clean fuels.


Subject(s)
Biodegradation, Environmental , Microalgae , Waste Disposal, Fluid , Wastewater , Wastewater/chemistry , Waste Disposal, Fluid/methods , Food Handling/methods , Water Pollutants, Chemical/analysis , Iron/chemistry , Hydrogen Peroxide/chemistry , Biological Oxygen Demand Analysis , Scenedesmus/growth & development
5.
Water Environ Res ; 96(1): e10981, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38264917

ABSTRACT

Green-synthesized iron nanoparticles (GAP-FeNP) were used as particle electrodes in a three-dimensional electro-Fenton (3DEF) process to accelerate the removal of hexavalent chromium [Cr (VI)]. Removal was evaluated by varying the pH (3.0, 6.0, and 9.0) and initial Cr (VI) concentrations (10, 30, and 50 mg/L) at 5 and 25 min. These results demonstrated that GAP-FeNP/3DEF treatment achieved more than 94% Cr (VI) removal under all tested conditions. Furthermore, it was observed that Cr (VI) removal exceeded 98% under pH 9.0 in all experimental parameters tested. The results of the response surface methodology (RSM) determined two optimal conditions: the first, characterized by a pH of 3.0, Cr (VI) concentration at 50 mg/L, and 25 min, yielded a Cr (VI) removal of 99.7%. The second optimal condition emerged at pH 9.0, with Cr (VI) concentrations of 10 mg/L and 5 min, achieving a Cr (VI) removal of 99.5%. This study highlights the potential of the GAP-FeNP to synergistically accelerate Cr (VI) removal by the 3DEF process, allowing faster elimination and expansion of the alkaline (pH 9.0) applicability. PRACTITIONER POINTS: The required time for >99% of Cr (VI) removal by the GAP-FeNP/3DEF process was shortened from 25 to 5 min. EF process with GAP-FeNP reduces the time necessary for Cr (VI) removal, which is 67% faster than conventional methods. EF process using GAP-FeNP removed >94% of Cr (VI) after 25 min for all initial Cr (VI) concentrations and pH treatments. Cr (VI) removal by the GAP-FeNP/3DEF process was >98% at a pH of 9.0, widening the solution pH applicability.


Subject(s)
Iron , Nanoparticles , Electrodes
6.
Environ Sci Pollut Res Int ; 30(56): 118736-118753, 2023 Dec.
Article in English | MEDLINE | ID: mdl-37917268

ABSTRACT

In this work, different iron-based cathode materials were prepared using two different approaches: a novel one-step approach, which involved the incorporation of iron oxide with Printex® L6 carbon/PTFE (PL6C/PTFE) on bare carbon felt (CF) and a two-step approach, where iron oxide is deposited onto CF previously modified with PL6C/PTFE. The results obtained from the physical characterization indicated that the presence of iron oxide homogeneously dispersed on the felt fibers with the CF 3-D network kept intact in the one-step approach; whereas the formation of iron oxide aggregates between the felt fibers for material obtained using the two-step approach. Among the iron oxide-based cathodes investigated, the iron-incorporated electrode exhibited the greatest efficiency in terms of the removal and mineralization of norfloxacin (NOR) under neutral pH (complete NOR removal in less than 30 min with around 50% mineralization after 90 min). The findings of this study show that the low cost and simple-to-prepare iron-modified carbon-based materials in HEF process led to the enhanced degradation of organic contaminants in aqueous solutions.


Subject(s)
Carbon , Water Pollutants, Chemical , Norfloxacin , Oxidation-Reduction , Water Pollutants, Chemical/analysis , Hydrogen Peroxide/chemistry , Iron/chemistry , Electrodes , Polytetrafluoroethylene/chemistry
7.
Chemosphere ; 345: 140466, 2023 Dec.
Article in English | MEDLINE | ID: mdl-37866502

ABSTRACT

This work describes the scientific and academic contributions of Professor Enric Brillas through the analysis of Social Network Analysis and data science. The study examines the research collaborations and co-authorship networks of Professor Brillas, indicating his active engagement and up-to-date collaborations with key co-authors, including Ignasi Sirés and Pere.L. Cabot. The analysis also reveals Professor Brillas' significant research focus on water treatment and related concepts such as oxidation-reduction, Fenton reactions, photoelectro-Fenton, and electrocatalysis. Furthermore, the most cited and recent articles by Professor Brillas are identified and discusses. Overall, the research demonstrates Professor Brillas' notable contributions to the field of electrochemical water treatment and highlights his ongoing research and collaborations in this area.


Subject(s)
Data Science , Social Network Analysis , Authorship , Oxidation-Reduction
8.
Article in English | MEDLINE | ID: mdl-37737947

ABSTRACT

Nowadays, the presence of persistent dissolved pollutants in water has received increasing attention due to their toxic effects on living organisms. Considering the limitations of conventional wastewater treatment processes for the degradation of these compounds, advanced oxidation processes such as electro-Fenton and sono-chemical process, as well as their combination, appear as potentially effective options for the treatment of wastewater contaminated with bio-recalcitrant pollutants. In view of the importance of the development of processes using real effluents, this review aims to provide a comprehensive perspective of sono-electro-Fenton-related processes applied for real wastewater treatment. In the first section, the fundamentals and effectiveness of both homogeneous and heterogeneous electro-Fenton approaches for the treatment of real wastewater are presented. While the second part of this work describes the fundamentals of ultrasound-based processes, the last section focuses on the coupling of the two methods for real wastewater treatment and on the effect of the main operational parameters of the process. On the basis of the information presented, it is suggested that sono-electro-Fenton processes substantially increase the efficiency of the treatment as well as the biodegradability of the treated wastewater. The combined effect results from mass transfer improvement, electrode cleaning and activation, water electrolysis, and the electro-Fenton-induced production of hydroxyl radicals. The information presented in this work is expected to be useful for closing the gap between laboratory-scale assays and the development of novel wastewater technologies.

9.
Chemosphere ; 339: 139666, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37532204

ABSTRACT

Today, water shortage problems around the world have forced the search for new treatment alternatives, in this context, electrochemical oxidation technology is a hopeful process for wastewater treatment, although it is still needed exploration of new efficient and economically viable electrode materials. In this way, mixed metal oxide anodes look like promising alternatives but their preparation is still a significant point to study, searching for finding low-cost materials to improve electrocatalytic efficiencies. In an exploration of this kind of highly efficient materials, this work presents the results obtained using an MMO Ti/IrO2-SnO2-Sb2O5 anode. All the prepared anodes exhibited excellent physical and electrochemical properties. The electrochemical oxidation of 100 mL and 200 mg L-1 Reactive Orange 84 (RO 84) diazo dye was studied using 3 cm2 of such synthesized anodes by applying current densities of 25, 50, and 100 mA cm-2. Faster and more efficient electrochemical oxidation occurred at 100 mA cm-2 with 50 mM of Na2SO4 + 10 mM NaCl as supporting electrolyte at pH 3.0. The degradation and mineralization processes of the above solution were enhanced with the electro-Fenton process with 0.05 mM Fe2+ and upgraded using photoelectron-Fenton with UVA light. This process yielded 91% COD decay with a low energy consumption of 0.1137 kWh (g COD)-1 at 60 min. The evolution of a final carboxylic acid like oxalic was followed by HPLC analysis. The Ti/IrO2-SnO2-Sb2O5 is then an efficient and low-cost anode for the photoelectro-Fenton treatment of RO 84 in a chloride and sulfate media.


Subject(s)
Ultraviolet Rays , Water Pollutants, Chemical , Titanium/chemistry , Hydrogen Peroxide/chemistry , Oxidation-Reduction , Electrodes , Water Pollutants, Chemical/chemistry , Electrochemical Techniques
10.
Chemosphere ; 336: 139209, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37315857

ABSTRACT

This study investigated the potential of a novel biomass-derived cork as a suitable catalyst after its modification with Fe@Fe2O3 for in-situ application in heterogeneous electro-Fenton (HEF) process for benzoquinone (BQ) elimination from water. No attempts on the application of modified granulated cork (GC) as a suspended heterogeneous catalyst in the HEF process for water treatment have been published yet. GC was modified by sonification approach in a FeCl3 + NaBH4 solution to reduce the ferric ions to metallic iron in order to obtain Fe@Fe2O3-modified GC (Fe@Fe2O3/GC). Results clearly demonstrated that this catalyst exhibited excellent electrocatalytic properties, such as a high conductivity as well as relatively high redox current and possessed several active sites for water depollution applications. Using Fe@Fe2O3/GC as catalyst in HEF, 100% of BQ removal was achieved in synthetic solutions by applying 33.3 mA cm-2 after 120 min. Different experimental conditions were tested to determine that best possible conditions can be as follow: 50 mmol L-1 Na2SO4 and 10 mg L-1 of Fe@Fe2O3/GC catalyst using Pt/carbon-PTFE air diffusion cell by applying 33.3 mA cm-2. Nevertheless, when Fe@Fe2O3/GC was used in the HEF approach to depollute real water matrices, no complete BQ concentration was removal achieved after 300 min of treatment, achieving between 80 and 95% of effectiveness.


Subject(s)
Iron , Water Pollutants, Chemical , Iron/chemistry , Carbon/chemistry , Hydrogen Peroxide/chemistry , Catalysis , Water Pollutants, Chemical/analysis , Oxidation-Reduction
11.
Chemosphere ; 323: 138254, 2023 May.
Article in English | MEDLINE | ID: mdl-36858121

ABSTRACT

H2S is a gaseous compound that contributes to air pollution. In this work, the electrochemical oxidation treatment of gaseous streams polluted with H2S is evaluated using a jet mixer and electrochemical cell device, in which the performance of electrolytic and electro-Fenton assisted absorption processes are compared. Results demonstrate the feasibility of both processes to remove H2S, reaching coulombic efficiencies of nearly 100% in the electrolytic assisted absorption, and 70-80% in the electro-Fenton assisted absorption. Aqueous solutions containing phosphate salts as electrolyte were found to be suitable as absorbents for the process. Efficiency in the cathodic production of H2O2 in these solutions using the experimental device was found to be as high as 32.8% (1.184 mgH2O2/min) at 12 °C and atmospheric pressure. Sequential formation of SO2 and SO3 is obtained by the oxidation of H2S contained in the gas. These species are hydrolysed, and a part remained in the absorbent as SO32- and SO42-, while the rest is dragged in the outlet gas. SO3 production is promoted by electrolytic assisted absorption and polysulphides by the electro-Fenton technology. Low concentrations of elemental sulphur are detected in the solid suspensions formed during the process.


Subject(s)
Gases , Water Pollutants, Chemical , Hydrogen Peroxide/chemistry , Electrolysis , Oxidation-Reduction , Electrodes , Water Pollutants, Chemical/chemistry
12.
Environ Res ; 213: 113552, 2022 10.
Article in English | MEDLINE | ID: mdl-35710024

ABSTRACT

Worldwide, most solid waste ends its life in landfill sites, which have a significant environmental impact in several respects. In particular, rainfall over landfill sites results in the production of an aqueous leachate containing compounds having low biodegradability, high toxicity, and a high organic load. For this reason, this study aims to investigate the applicability of electro-Fenton (EF) and photoelectro-Fenton (PEF) processes as alternative for treating a local landfill effluent with high organic content (chemical oxygen demand (COD) = 2684.7 mg-O2 L -1) in a continuous-flow reactor (using, for first time, this kind of system with higher electrodes area of 35 cm2) using boron-doped diamond anode (Nb/BDD) and a carbon felt cathode (FC) electrodes. The effects of current density j (30, 60 and 90 mA cm-2) and UV radiation wavelength (UVA and UVC) were studied to evaluate the treatment efficiency as well as the energy consumption. Results clearly showed that, the best efficiencies removing organic matter, in terms of COD, were about 66%, 68% and 89% with an energy consumption of only 19.41, 17.61 and 17.59 kWh kg COD-1 for EF, PEF-UVA and PEF-UVC respectively, at 90 mA cm-2 after 4 h of operation. The treatment of this kind of effluent produced organic and inorganic by-products, the acetic and formic acids as well as NO2-, NO3-, and NH4+, being assessed their concentrations.


Subject(s)
Water Pollutants, Chemical , Diamond , Hydrogen Peroxide/chemistry , Iron/chemistry , Oxidation-Reduction , Water Pollutants, Chemical/chemistry
13.
Chemosphere ; 303(Pt 1): 134883, 2022 Sep.
Article in English | MEDLINE | ID: mdl-35577132

ABSTRACT

Paracetamol (PCT), also known as acetaminophen, is a drug used to treat fever and mild to moderate pain. After consumption by animals and humans, it is excreted through the urine to the sewer systems, wastewater treatment plants, and other aquatic/natural environments. It has been detected in trace amounts in effluents of wastewater plant treatments, sewage sludge, hospital wastewaters, surface waters, and drinking water. PCT can cause genetic code damage, oxidative degradation of lipids, and denaturation of protein in cells, and its toxicity has been well-proven in bacteria, algae, macrophytes, protozoan, and fishes. To avoid its harmful health problems over living beings, powerful Fenton and Fenton-based treatments as pre-eminent advanced oxidation processes (AOPs) have been developed because of the inefficient treatment by conventional treatments. This paper presents a comprehensive and critical review over the application of such Fenton technologies to remove PCT from natural waters, synthetic wastewaters, and real wastewaters. The characteristics and main results obtained using Fenton, photo-Fenton, electro-Fenton, and photoelectro-Fenton are described, making special emphasis in the oxidative action of the generated reactive oxygen species. Hybrid processes based on the coupling with ultrasounds, gamma radiation, photocatalysis, photoelectrocatalysis, zero-valent iron-activated persulfate, adsorption, and microbial fuel cells, are analyzed. Sequential treatments involving the initiation with plasma gliding arc discharge and post-biological process are detailed. Comparative results with other available AOPs are also described and discussed. Finally, 13 aromatic by-products and 9 short-linear aliphatic carboxylic acid detected during the PCT removal by Fenton and Fenton-based processes are reported, with the proposal of three parallel pathways for its initial degradation.


Subject(s)
Water Pollutants, Chemical , Water Purification , Acetaminophen , Animals , Hydrogen Peroxide/metabolism , Oxidation-Reduction , Wastewater , Water , Water Purification/methods
14.
Sci Total Environ ; 827: 154348, 2022 Jun 25.
Article in English | MEDLINE | ID: mdl-35257780

ABSTRACT

Pharmaceutical and personal care products (PPCPs) are part of the emerging contaminants (ECs) in the environment due to their known or suspected adverse effects in aquatic and terrestrial organisms, as well as in human health. Presence of PPCPs in aquatic and terrestrial ecosystems has been mainly attributed to the effluents of wastewater treatment plants (WWTPs). Although several PPCPs have been detected in wastewater, their removal from wastewater via biological processes is limited. Removal of PPCPs depends on their chemical structure, concentration, solubility, and technology used to treat the wastewater. Electrochemical Advanced Oxidation Processes (EAOPs) are some of the most sought-after methods for dealing with organic pollutants in water including PPCPs, due to generation of strong oxidants such as •OH, H2O2 and O3- by using directly or indirectly electrochemical technology. This review is focused on the removal of main PPCPs via EAOPs such as, anodic oxidation, electro-Fenton, photoelectron-Fenton, solar photoelectron-Fenton, photoelectrocatalysis and sonoelectrochemical processes. Although more than 40 PPCPs have been identified through different analytical approaches, antibiotics, anti-inflammatory and antifungal are the main categories of PPCPs detected in different water matrices. Application of EAOPs has been centered in the removal of antibiotics and analgesics of high consumption by using model media, e.g. Na2SO4. Photoelectrocatalysis and Electro-Fenton processes have been the most versatile EAOPs applied for PPCPs removal under a wide range of operating conditions and a variety of electrodes. Although EAOPs have gained significant scientific interest due to their effectiveness, low environmental impact, and simplicity, further research about the removal of PPCPs and their by-products under realistic concentrations and media is needed. Moreover, mid-, and long-term experiments that evaluate EAOPs performance will provide knowledge about key parameters that allow these technologies to be scaled and reduce the potential risk of PPCPs in aquatic and terrestrial ecosystem.


Subject(s)
Cosmetics , Water Pollutants, Chemical , Anti-Bacterial Agents , Cosmetics/analysis , Ecosystem , Humans , Hydrogen Peroxide , Pharmaceutical Preparations , Rivers , Waste Disposal, Fluid/methods , Wastewater/chemistry , Water , Water Pollutants, Chemical/analysis
15.
Molecules ; 26(18)2021 Sep 21.
Article in English | MEDLINE | ID: mdl-34577184

ABSTRACT

Metal-organic-frameworks (MOFs) are emerging materials used in the environmental electrochemistry community for Faradaic and non-Faradaic water remediation technologies. It has been concluded that MOF-based materials show improvement in performance compared to traditional (non-)faradaic materials. In particular, this review outlines MOF synthesis and their application in the fields of electron- and photoelectron-Fenton degradation reactions, photoelectrocatalytic degradations, and capacitive deionization physical separations. This work overviews the main electrode materials used for the different environmental remediation processes, discusses the main performance enhancements achieved via the utilization of MOFs compared to traditional materials, and provides perspective and insights for the further development of the utilization of MOF-derived materials in electrified water treatment.

16.
J Environ Sci Health B ; 56(7): 670-674, 2021.
Article in English | MEDLINE | ID: mdl-34157949

ABSTRACT

Paraquat is resistant to degradation by conventional treatments, being necessary to use treatments with greater effectiveness, such as advanced oxidative processes. In this work, different advanced oxidative processes were applied (Fenton, electro-Fenton, photoelectro-oxidation and photoelectro-Fenton) employing oxide electrodes to degrade Gramoxone, a commercial herbicide that contains paraquat in its composition. The degradation and formation of by-products were accompanied by high performance liquid chromatography, total organic carbon (TOC) and chemical oxygen demand (COD). The results showed that the photoelectro-Fenton process was the most efficient due to the synergistic effect, reaching 79% degradation of the initial compound and 82% and 71% removal of TOC and COD, respectively. After the application of the electro-Fenton and photoelectro-Fenton oxidation processes, short-chain carboxylic acids such as succinic acid, oxalic acid, acetic acid and formic acid were identified as by-products of the oxidation of Gramoxone. The results were satisfactory and deserve to be highlighted, as a commercial formulation was used, making the scenario more realistic.


Subject(s)
Herbicides , Water Pollutants, Chemical , Electrodes , Hydrogen Peroxide , Oxidation-Reduction , Oxidative Stress , Paraquat
17.
Chemosphere ; 274: 129683, 2021 Jul.
Article in English | MEDLINE | ID: mdl-33540303

ABSTRACT

Amitriptyline (AMT) is the most widely used tricyclic antidepressant and is classified as a recalcitrant emergent contaminant because it has been detected in different sources of water. Its accumulation in water and soil represents a risk for different living creatures. To remove amitriptyline from wastewater, the Advanced Oxidation Processes (AOPs) stands up as an interesting option since generate highly oxidized species as hydroxyl radicals (OH) by environmentally friendly mechanism. In this work, the oxidation and mineralization of AMT solution have been comparatively studied by 3 Electrochemical AOPs (EAOPs) where the OH is produced by anodic oxidation of H2O (AO-H2O2), or by electro-Fenton (EF) or photoelectro-Fenton (PEF). PEF process with a BDD anode showed the best performance for degradation and mineralization of this drug due to the synergistic action of highly reactive physiosorbed BDD (OH), homogeneous OH and UVA radiation. This process achieved total degradation of AMT at 50 min of electrolysis and 95% of mineralization after 360 min of treatment with 0.5 mmol L-1 Fe2+ at 100 mA cm-2. Six aromatic intermediates for the drug mineralization were identified in short time of electrolysis by GC-MS, including a chloroaromatic by-product formed from the attack of active chlorine. Short-chain carboxylic acids like succinic, malic, oxalic and formic acid were quantified by ion-exclusion HPLC. Furthermore, the formation of NO3- ions was monitored. Finally, the organic intermediates identified by chromatographic techniques were used to propose the reaction sequence for the total mineralization of AMT.


Subject(s)
Hydrogen Peroxide , Water Pollutants, Chemical , Amitriptyline , Antidepressive Agents , Electrochemical Techniques , Electrodes , Oxidation-Reduction
18.
Environ Sci Pollut Res Int ; 28(19): 23929-23945, 2021 May.
Article in English | MEDLINE | ID: mdl-33398742

ABSTRACT

A simple, efficient, environmentally friendly, and inexpensive synthesis route was developed to obtain a magnetic nano-hybrid (GH) based on graphene and cobalt ferrite. Water with a high content of natural organic matter (NOM) was used as solvent and a source of carbon. The presence of NOM in the composition of GH was confirmed by FTIR and Raman spectroscopy, which evidenced the formation of graphene, as also corroborated by XRD analyses. The diffractograms and TEM images showed the formation of a hybrid nanomaterial composed of graphene and cobalt ferrite, with crystallite and particle sizes of 0.83 and 4.0 nm, respectively. The heterogeneous electro-Fenton process (EF-GH) achieved 100% degradation of bisphenol A (BPA) in 50 min, with 80% mineralization in 7 h, at pH 7, using a current density of 33.3 mA cm-2. The high catalytic performance was achieved at neutral pH, enabling substantial reduction of the costs of treatment processes. This work contributes to understanding the role of NOM in the synthesis of a magnetic nano-hybrid based on graphene and cobalt ferrite, for use in heterogeneous catalysis. This nano-hybrid has excellent potential for application in the degradation of persistent organic pollutants found in aquatic environments.


Subject(s)
Graphite , Water Pollutants, Chemical , Benzhydryl Compounds , Catalysis , Cobalt , Ferric Compounds , Hydrogen Peroxide , Iron , Oxidation-Reduction , Phenols , Water Pollutants, Chemical/analysis
19.
Environ Sci Pollut Res Int ; 28(19): 23984-23994, 2021 May.
Article in English | MEDLINE | ID: mdl-33405147

ABSTRACT

This work deals with the theoretical approach of biodegradability, lipophilicity, and physiological activity of VAL and four degradation products (DPs) detected after 20 min of the photo-electro-Fenton (PEF) process. The biodegradability calculation, taking into account the change in the theoretical oxygen demand, showed that the four DPs had a more negative value than VAL, indicating that they are more susceptible to oxidation. However, these results do not imply more accessible biotransformation pathways than VAL, as observed using the EAWAG-BBD program, through which neutral biotransformation pathway prediction for VAL and DPs was made. Subsequently, by calculating the theoretical lipophilicity of the molecules (log P), the theoretical toxicity of the DPs was proposed, where the DPs had log P values between 1 and 3, lower values than those of VAL (log P = 4), indicating that DPs could be less toxic than the original compound (VAL). Both results suggest that VAL degradation (by photo-electro-Fenton process proposed) yields a positive effect on the environment. Finally, when molecular dynamic simulations were carried out, it was observed that DP1, DP2, and DP3 maintained similar interactions to those of VAL with the binding site of the AT1R. DP4 did not show any interaction. These results indicated that, despite the presence of DPs, generated after 20 min of the treatment, they could not exert a physiological activity in any organism the same way that does VAL.


Subject(s)
Hydrogen Peroxide , Water Pollutants, Chemical , Computers , Iron , Oxidation-Reduction , Receptor, Angiotensin, Type 1 , Valsartan , Water Pollutants, Chemical/analysis
20.
Environ Sci Pollut Res Int ; 28(19): 23699-23706, 2021 May.
Article in English | MEDLINE | ID: mdl-33010016

ABSTRACT

Vinasse wastewater from tequila industry that has been conventionally treated is usually characterized by a chemical oxygen demand (COD) above 150 mg L-1, which is the maximum content permitted for discharge by Mexican Regulation. In order to increase the wastewater quality, different processes were applied, and from the experimental results, the advantages and limitations were analyzed. In this way, although Fenton experiments showed acceptable COD removal efficiencies (79-90%), operation as well as cost limit its adoption as a viable technology. Therefore, additional experiments explored electro-Fenton (EF) as well as adsorption coupled to EF in a tubular reactor. The corresponding data revealed that there was no additional increase in COD removal performance probably due to the low oxygen solubility in the electrolytic solution and the high pH that prevents the existence of Fe2+ ions necessary for the Fenton mixture. In view of these results, when an activated carbon (AC) filter was coupled to polarization at current densities between 0.5 and 2 mA cm-2, removal efficiencies from 71 to 81%, corresponding to final COD of 78 to 33 mg L-1, were achieved. Also, the adsorbent surface was continuously regenerated, promoting a more efficient adsorption and a longer service life for the AC filter. In this case, by using a current density of 0.5 mA cm-2, COD was reduced to sufficiently small values for discharge into natural water bodies, maintaining low energy consumption and therefore acceptable operation costs.


Subject(s)
Wastewater , Water Pollutants, Chemical , Adsorption , Biological Oxygen Demand Analysis , Hydrogen Peroxide , Oxidation-Reduction , Waste Disposal, Fluid
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