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1.
Small ; 19(33): e2301540, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37093555

RESUMEN

Hydrogen peroxide (H2 O2 ) is essential in oxidative stress and signal regulation of organs of animal body. Realizing in vitro quantification of H2 O2 released from organs is significant, but faces challenges due to short lifetime of H2 O2 and complex bio-environment. Herein, rationally designed and constructed a photoelectrochemical (PEC) sensor for in vitro sensing of H2 O2 , in which atomically dispersed iron active sites (Hemin) modified graphdiyne (Fe-GDY) serves as photoelectrode and catalyzes photo-electro-Fenton process. Sensitivity of Fe-GDY electrode is enhanced 8 times under illumination compared with dark condition. The PEC H2 O2 sensor under illumination delivers a wide linear range from 0.1 to 48 160 µm and a low detection limit of 33 nm, while demonstrating excellent selectivity and stability. The high performance of Fe-GDY is attributed to, first, energy levels matching of GDY and Hemin that effectively promotes the injection of photo-generated electrons from GDY to Fe3+ for reduced Fe2+ , which facilitates the Fe3+ /Fe2+ cycle. Second, the Fe2+ actively catalyzes H2 O2 to OH- through the Fenton process, thereby improving the sensitivity. The PEC sensor demonstrates in vitro quantification of H2 O2 released from different organs, providing a promising approach for molecular sensing and disease diagnosis in organ levels.

2.
Environ Sci Technol ; 57(41): 15693-15702, 2023 10 17.
Artículo en Inglés | MEDLINE | ID: mdl-37791801

RESUMEN

Metals usually served as the active sites of the heterogeneous bifunctional electro-Fenton reaction, which faced the challenge of poor stability under acidic or even neutral conditions. Exploring a metal-free heterogeneous bifunctional electro-Fenton catalyst can effectively solve the above problems. In this work, a stable metal-free heterogeneous bifunctional boron-modified porous carbon catalyst (BTA-1000) was synthesized. For the BTA-1000 catalyst, the yield of H2O2 (294 mg/L) significantly increased. The degradation rate of phenol by BTA-1000 (0.242 min-1) increased by an order of magnitude, compared with the porous carbon catalyst (0.0105 min-1). The BTA catalyst could rapidly degrade industrial dye wastewater, and its specific energy consumption was 5.52 kW h kg-1 COD-1, lower than that in previous reports (6.38-7.4 kW h kg-1 COD-1). DFT and XPS revealed that C═O and -BC2O groups jointly promoted the generation of H2O2, and the -BCO2 group played dominant roles in the generation of •OH because the oxygen atom near the electron-giving groups (-BCO2 group) facilitated the formation of hydrogen bond and H2O2 adsorption. This work gained deep insights into the reaction mechanism of the boron-modified porous carbon catalyst, which helped to guide the development of metal-free heterogeneous bifunctional electro-Fenton catalysts.


Asunto(s)
Peróxido de Hidrógeno , Contaminantes Químicos del Agua , Peróxido de Hidrógeno/química , Contaminantes Orgánicos Persistentes , Boro , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis , Electrodos , Carbono , Metales , Catálisis
3.
J Environ Manage ; 348: 119328, 2023 Dec 15.
Artículo en Inglés | MEDLINE | ID: mdl-37857210

RESUMEN

Discharge of endocrine-disrupting compounds such as methylparaben (MePa) into natural water bodies deteriorates the aquatic ecosystem. In this regard, electrochemical oxidation (EO) and electro-Fenton (EF) processes are acknowledged as effective methods to eliminate biorecalcitrant compounds from different wastewater matrices. In these systems, the H2O2-producing ability of carbon-based cathodes is put to advantage for producing homogenous hydroxyl radicals by simulating Fenton's reaction, which dramatically augments the contaminant removal efficiency. However, commercial carbon based cathodes are not economically affordable, especially for voluminous treatment. Hence in the present work, waste-derived carbonised coconut shell (CCS) monolith was employed as a cathode in EO and EF treatment of MePa. Almost the entire MePa with initial concentration of 10 mg/L was removed in 60 min by EO and 45 min by EF process at neutral pH, applied current density of 7.5 mA/cm2, NaCl concentration of 1.0 g/L and 10 mg/L of Fe2O3 dosing. The MePa removal efficiency of the CCS cathode-fitted system after 60 min was better than the commercial graphite plate and Ti-based mixed metal oxide employing system due to higher H2O2 electrosynthesis (H2O2 = 9.0 ± 0.6 mg/L after 60 min). Moreover, the same setup was used for treating 10 mg/L of MePa-spiked real sewage and demonstrated MePa and total organic carbon removal efficiency of 80.16 ± 2.31% and 37.42 ± 3.50%, respectively, in 45 min. Further, the CCS-mediated EF treatment achieved >90% removal of MePa for eight continuous batch cycles and recorded a current density drop of just 0.23% per cycle. The degradation pathway and toxicity assessment of the intermediates using the Ecological Structure Activity Relationships (ECOSAR) tool supported the eco-friendliness of the current treatment scheme.


Asunto(s)
Carbono , Contaminantes Químicos del Agua , Cocos , Peróxido de Hidrógeno/química , Ecosistema , Electrodos , Contaminantes Químicos del Agua/química , Oxidación-Reducción
4.
Angew Chem Int Ed Engl ; 62(52): e202314414, 2023 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-37946623

RESUMEN

The integration of highly active single atoms (SAs) and atom clusters (ACs) into an electrocatalyst is critically important for high-efficiency two-electron oxygen reduction reaction (2e- ORR) to hydrogen peroxide (H2 O2 ). Here we report a tandem impregnation-pyrolysis-etching strategy to fabricate the oxygen-coordinated Fe SAs and ACs anchored on bacterial cellulose-derived carbon (BCC) (FeSAs/ACs-BCC). As the electrocatalyst, FeSAs/ACs-BCC exhibits superior electrocatalytic activity and selectivity toward 2e- ORR, affording an onset potential of 0.78 V (vs. RHE) and a high H2 O2 selectivity of 96.5 % in 0.1 M KOH. In a flow cell reactor, the FeSAs/ACs-BCC also achieves high-efficiency H2 O2 production with a yield rate of 12.51±0.18 mol gcat -1 h-1 and a faradaic efficiency of 89.4 %±1.3 % at 150 mA cm-2 . Additionally, the feasibility of coupling the produced H2 O2 and electro-Fenton process for the valorization of ethylene glycol was explored in detail. The theoretical calculations uncover that the oxygen-coordinated Fe SAs effectively regulate the electronic structure of Fe ACs which are the 2e- ORR active sites, resulting in the optimal binding strength of *OOH intermediate for high-efficiency H2 O2 production.

5.
Environ Res ; 197: 111144, 2021 06.
Artículo en Inglés | MEDLINE | ID: mdl-33844966

RESUMEN

The disadvantages of limited working pH range and poor stability have hindered the practical application of traditional electro-Fenton process. In this research, a novel heterogeneous electro-Fenton (HEF) process with FeIIFeIII layered double hydroxide/carbon felt (FeIIFeIII LDH/CF) as cathode was developed for the rapid destruction of ciprofloxacin (CIP) in bulk solution. Effects of crucial influencing factors (initial pH, current intensity) on CIP degradation were investigated. Results indicated that FeIIFeIII LDH/CF cathode was efficient for CIP degradation (88.11%). Furthermore, CIP degradation performance in HEF could remain stable over wide range of pH (pH 3-9). The catalytic degradation of CIP in HEF process might be a combined effect of homogeneous EF reaction, anodic oxidation, and surface catalysis process via≡FeII/≡FeIII cycle. Possible degradation pathways were proposed. The results suggested that FeIIFeIII LDH/CF cathode showed great application potential for CIP degradation.


Asunto(s)
Ciprofloxacina , Contaminantes Químicos del Agua , Carbono , Fibra de Carbono , Electrodos , Compuestos Férricos , Peróxido de Hidrógeno , Hidróxidos , Oxidación-Reducción
6.
Molecules ; 25(24)2020 Dec 12.
Artículo en Inglés | MEDLINE | ID: mdl-33322793

RESUMEN

This paper studies the degradation of methiocarb, a highly hazardous pesticide found in waters and wastewaters, through an electro-Fenton process, using a boron-doped diamond anode and a carbon felt cathode; and evaluates its potential to reduce toxicity towards the model organism Daphnia magna. The influence of applied current density and type and concentration of added iron source, Fe2(SO4)3·5H2O or FeCl3·6H2O, is assessed in the degradation experiments of methiocarb aqueous solutions. The experimental results show that electro-Fenton can be successfully used to degrade methiocarb and to reduce its high toxicity towards D. magna. Total methiocarb removal is achieved at the applied electric charge of 90 C, and a 450× reduction in the acute toxicity towards D. magna, on average, from approximately 900 toxic units to 2 toxic units, is observed at the end of the experiments. No significant differences are found between the two iron sources studied. At the lowest applied anodic current density, 12.5 A m-2, an increase in iron concentration led to lower methiocarb removal rates, but the opposite is found at the highest applied current densities. The highest organic carbon removal is obtained at the lowest applied current density and added iron concentration.


Asunto(s)
Biodegradación Ambiental , Insecticidas/metabolismo , Metiocarb/metabolismo , Contaminantes Químicos del Agua/metabolismo , Animales , Daphnia/efectos de los fármacos , Ecotoxicología/métodos , Electroquímica/métodos , Electrodos , Insecticidas/química , Insecticidas/toxicidad , Metiocarb/química , Metiocarb/toxicidad
7.
J Environ Manage ; 210: 328-337, 2018 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-29367141

RESUMEN

Treatment of stabilized landfill leachate is a great challenge due to its poor biodegradability. Present study made an attempt to treat this wastewater by combining electro-Fenton (E-Fenton) and biological process. E-Fenton treatment was applied prior to biological process to enhance the biodegradability of leachate, which will be beneficial for the subsequent biological process. This study also investigates the efficiency of iron molybdophosphate (FeMoPO) nanoparticles as a heterogeneous catalyst in E-Fenton process. The effects of initial pH, catalyst dosage, applied voltage and electrode spacing on Chemical Oxygen Demand (COD) removal efficiency were analyzed to determine the optimum conditions. Heterogeneous E-Fenton process gave 82% COD removal at pH 2, catalyst dosage of 50 mg/L, voltage 5 V, electrode spacing 3 cm and electrode area 25 cm2. Combined E-Fenton and biological treatment resulted an overall COD removal of 97%, bringing down the final COD to 192 mg/L.


Asunto(s)
Análisis de la Demanda Biológica de Oxígeno , Contaminantes Químicos del Agua , Fenómenos Biológicos , Peróxido de Hidrógeno , Oxidación-Reducción
8.
Environ Monit Assess ; 190(6): 340, 2018 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-29748751

RESUMEN

Since 2,4-dichlorophenol (2,4-DCP) as a priority pollutant is used in numerous industrial processes, its removal from the aqueous environment is of utmost importance and desire. Herein, the authors describe an electrochemical treatment process for efficient removal of 2,4-DCP from aqueous solutions using electro-Fenton (EF) process. Response surface methodology (RSM) was applied to optimize the operating parameters. Analysis of variance (ANOVA) confirmed the significance of the predicted model. The effect of independent variables on the removal of 2,4-DCP was investigated and the best removal efficiency of 98.28% achieved under the optimal experimental condition including initial pH of 3, H2O2 dosage of 80 µL, initial 2,4-DCP concentration of 3.25 mg L-1, current density of 3.32 mA cm-2, and inter-electrode distance of 5.04 cm. The predicted removal efficiency was in satisfactory agreement with the obtained experimental removal efficiency of 99.21%. According to the obtained polynomial model, H2O2 dosage revealed the most significant effect on degradation process. The kinetic investigation revealed that the first-order model with the correlation coefficient of 0.9907 and rate constant (Kapp) of 0.831 min-1 best fitted with the experimental results. Generation of the hydroxyl radicals throughout the EF process controlled the degradation process.


Asunto(s)
Clorofenoles/química , Monitoreo del Ambiente/métodos , Restauración y Remediación Ambiental/métodos , Peróxido de Hidrógeno/química , Aguas Residuales/análisis , Contaminantes Químicos del Agua/química , Electrodos , Radical Hidroxilo/química , Hierro/química , Oxidación-Reducción , Fenoles/química
9.
Artículo en Inglés | MEDLINE | ID: mdl-27726493

RESUMEN

The hydroxyl radical generation in an electro-Fenton process with a gas-diffusion electrode which is strongly linked with electro-chemical generation of hydrogen peroxide and iron redox cycle was studied. The OH radical generation subsequent to electro-chemical generations of H2O2 was examined under the constant potential in the range of Fe2+ dosage from 0 to 1.0 mM. The amount of generated OH radical initially increased and gradually decreased after the maximum was reached. The initial rate of OH radical generation increased for the Fe2+ dosage <0.25 mM and at higher Fe2+ dosages remained constant. At higher Fe2+ dosages the precipitation of Fe might inhibit the enhancement of OH radical generation. The experiments for decolorization and total organic carbon (TOC) removal of azo-dye Orange II by the electro-Fenton process were conducted and the quick decolorization and slow TOC removal of Orange II were found. To quantify the linkages of OH radical generation with dynamic behaviors of electro-chemically generated H2O2 and iron redox cycle and to investigate effects of OH radical generation on the decolorization and TOC removal of Orange II, novel reaction kinetic models were developed. The proposed models could satisfactory clarify the linkages of OH radical generation with electro-chemically generated H2O2 and iron redox cycle and simulate the decolorization and TOC removal of Orange II by the electro-Fenton process.


Asunto(s)
Compuestos Azo/química , Bencenosulfonatos/química , Colorantes/química , Peróxido de Hidrógeno/química , Radical Hidroxilo/química , Hierro/química , Contaminantes Químicos del Agua/química , Difusión , Electrodos , Cinética , Oxidación-Reducción
10.
J Environ Manage ; 165: 96-105, 2016 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-26413803

RESUMEN

This study aims to investigate the effectiveness of the electro-Fenton process on the removal of a second generation of fluoroquinolone, enoxacin. The electrochemical reactor involved a carbon-felt cathode and a platinum anode. The influence of some experimental parameters, namely the initial enoxacin concentration, the applied current intensity and the Fe(II) amount, was examined. The degradation of the target molecule was accompanied by an increase of the biodegradability, assessed from the BOD5 on COD ratio, which increased from 0 before treatment until 0.5 after 180 min of electrolysis at 50 mg L(-1) initial enoxacin concentration, 0.2 mmol L(-1) Fe(II) concentration and 300 mA applied current intensity. TOC and COD time-courses were also evaluated during electrolysis and reached maximum residual yields of 54% and 43% after 120 min of treatment, respectively. Moreover, a simultaneous generation of inorganic ions (fluorides, ammonium and nitrates) were observed and 3 short chain carboxylic acids (formic, acetic and oxalic acids) were identified and monitored during 180 min of electrolysis. By-products were identified according to UPLC-MS/MS results and a degradation pathway was proposed.


Asunto(s)
Antibacterianos/química , Enoxacino/química , Contaminantes Químicos del Agua/química , Ácido Acético/química , Antibacterianos/metabolismo , Biodegradación Ambiental , Análisis de la Demanda Biológica de Oxígeno , Carbono/química , Técnicas Electroquímicas/instrumentación , Técnicas Electroquímicas/métodos , Electrodos , Electrólisis , Enoxacino/metabolismo , Fluoruros/química , Hierro/química , Nitratos , Platino (Metal) , Espectrometría de Masas en Tándem , Contaminantes Químicos del Agua/metabolismo
11.
Chemistry ; 21(20): 7611-20, 2015 May 11.
Artículo en Inglés | MEDLINE | ID: mdl-25829133

RESUMEN

Development of novel nanocatalysts for the highly efficient in situ synthesis of H2 O2 from H2 and O2 in the electro-Fenton (EF) process has potential for the remediation of water pollution. In this work, AuPd/carbon nanotube (CNT) nanocatalysts were successfully synthesized by the facile aggregation of AuPd bimetals on CNTs. Characterization by X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy indicated that pure AuPd bimetallic heterogeneous nanospheres (≈20 nm) were well dispersed outside the CNTs, which resulted in better catalytic performance than Pd/CNTs alone: 0.36 M H2 O2 was synthesized; 0.05 M Fe(2+) optimally initiated the EF process due to the superior in situ Fe(2+) regeneration; and the organic pollutant removal reached 100 % at 37 min, with a pseudo-first-order kinetic constant k1 =0.051 min(-1) . Moreover, structural insights before/after catalysis revealed that Au strengthened the construction of the nanocrystals, avoided negative deactivation caused by AuPd agglomeration, and immobilized the active Pd(111). The catalytic stability of AuPd/CNTs over ten cycles implied long durability and promising applications of this material.

12.
Environ Technol ; 36(13-16): 1924-32, 2015.
Artículo en Inglés | MEDLINE | ID: mdl-25666104

RESUMEN

Organic compound is the main pollutant in industrial effluent. Conventional wastewater treatment processes are inefficient for the removal of toxic or non-biodegradable organic pollutants. Advanced electrochemical depollution is a very efficient and economic method, suitable when the wastewater contains toxic and recalcitrant organic pollutants. The aim of the present study was to investigate the application of the electro-Fenton (EF) process for the degradation and mineralization of a stable oil-in-water emulsion (0.01% in v/v). The effects of operating parameters such as cathode material (graphite, Ti/Pt and steel), nature (Na2SO4, NaNO3 and NaCl) and dose of electrolyte (25-75 mM), initial ferrous ions concentration (1-75 mM), current intensity (0.1-0.2 A) and operating time, on chemical oxygen demand (COD) removal efficiency, were studied. Results showed that the EF method can be used efficiently for the degradation of stable cutting oil emulsion. For considered initial conditions (bubbling compressed air at 1 L/min, 0.15 A, pH 3, [Na2SO4]=0.05 M, [FeSO4]=0.015 M, COD0=400 mg O2/L), the best removal efficiencies were obtained under the following conditions: graphite as cathode material, 180 min for treatment duration and 0.05 M [Na2SO4]. For these conditions, treatment of 250 mL of emulsion led to 93.6% of cutting fluid mineralization, which correspond to 25 mg O2/L of final COD, 19 kWh/m3 of treated wastewater and 24.039 kWh/kg of COD removal.


Asunto(s)
Peróxido de Hidrógeno/química , Hierro/química , Minerales/aislamiento & purificación , Aceites/aislamiento & purificación , Contaminantes Químicos del Agua/aislamiento & purificación , Purificación del Agua/métodos , Electroquímica/métodos , Electrólisis/métodos , Peróxido de Hidrógeno/efectos de la radiación , Hierro/efectos de la radiación , Minerales/química , Aceites/química , Aceites/efectos de la radiación , Dosis de Radiación , Aguas Residuales/química , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/efectos de la radiación
13.
Sci Total Environ ; 953: 176110, 2024 Nov 25.
Artículo en Inglés | MEDLINE | ID: mdl-39265676

RESUMEN

A bimetallic FeCu/NC core-shell catalyst, consisting in nanoparticles where zero-valent Fe and Cu atoms, slightly oxidized on their surface, are encapsulated by carbon has been successfully prepared by modifying the synthesis route of MIL(Fe)-88B. FeCu/NC possessed well-balanced textural and electrochemical properties. According to voltammetric responses, in-situ Fe(III) reduction to Fe(II) by low-valent Cu was feasible, whereas the high double-layer capacitance confirmed the presence of a great number of electroactive sites that was essential for continuous H2O2 activation to •OH via Fenton's reaction. Electrochemical impedance and distribution of relaxation times (DRT) analysis informed about the strong leaching resistance of FeCu/NC. To validate the promising features of this catalyst, the advanced oxidation of the antihypertensive lisinopril (LSN) was investigated for the first time. The heterogeneous electro-Fenton (HEF) treatment of 16.1 mg L-1 LSN solutions was carried out in a DSA/air-diffusion cell. At pH 3, complete degradation was achieved within 6 min using only 0.05 g L-1 FeCu/NC; at near-neutral pH, 100 % removal was also feasible even in actual urban wastewater, requiring 60-75 min. The FeCu/NC catalyst demonstrated high stability, still maintaining 86.5 % of degradation efficiency after 5 cycles and undergoing low iron leaching. It outperformed the monometallic (Fe/NC and Cu/NC) catalysts, which is explained by the Cu(0)/Cu(I)-catalyzed Fe(II) regeneration mechanism that maintains the Fenton's cycle. LC-MS/MS analysis allowed the identification of two main primary LSN by-products. It can then be concluded that the FeCu/NC-based HEF process merits to be further scaled up for wastewater treatment.

14.
ChemSusChem ; : e202401758, 2024 Sep 09.
Artículo en Inglés | MEDLINE | ID: mdl-39250234

RESUMEN

The high cost and often complex synthesis procedure of new highly selective electrocatalysts (particularly those based on noble metals) for H2O2 production are daunting obstacles to penetration of this technology into the wastewater treatment market. In this work, a simple direct thermal method has been employed to synthesize Sn-doped carbon electrocatalysts, which showed an electron transfer number of 2.04 and outstanding two-electron oxygen reduction reaction (ORR) selectivity of up to 98.0%. Physicochemical characterization revealed that this material contains 1.53% pyrrolic nitrogen, which is beneficial for the production of H2O2, and -C≡N functional group, which is advantageous for H+ transport. Moreover, the high volume ratio of mesopores to micropores is known to favor the quick escape of H2O2 from the electrode surface, thus minimizing its further oxidation. A purpose-made gas-diffusion electrode (GDE) was prepared, yielding 20.4 mM H2O2 under optimal electrolysis conditions. The drug diphenhydramine was selected for the first time as model organic pollutant to evaluate the performance of an electrochemical advanced oxidation process. In conventional electro-Fenton process (pH 3), complete degradation was achieved in only 15 min at 10 mA cm-2, whereas at natural pH 5.9 and 33.3 mA cm-2, almost overall drug removal was reached in 120 min.

15.
Water Environ Res ; 96(1): e10981, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-38264917

RESUMEN

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.


Asunto(s)
Hierro , Nanopartículas , Electrodos
16.
Chemosphere ; 364: 143249, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-39233296

RESUMEN

Conventional electro-Fenton (EF) process at acidic pH ∼3 is recognized as a highly effective strategy to degrade organic pollutants; however, homogeneous metal catalysts cannot be employed in more alkaline media. To overcome this limitation, pyrolytic derivatives from metal-organic frameworks (MOFs) have emerged as promising heterogeneous catalysts. Cu-based MOFs were prepared using trimesic acid as the organic ligand and different pyrolysis conditions, yielding a set of nano-Cu/C catalysts that were analyzed by conventional methods. Among them, XPS revealed the surface of the Cu/C-A2-Ar/H2 catalyst was slightly oxidized to Cu(I) and, combined with XRD and HRTEM data, it can be concluded that the catalyst presents a core-shell structure where metallic copper is embedded in a carbon layer. The antihistamine diphenhydramine (DPH), spiked into either synthetic Na2SO4 solutions or actual urban wastewater, was treated in an undivided electrolytic cell equipped with a DSA-Cl2 anode and a commercial air-diffusion cathode able to electrogenerate H2O2. Using Cu/C as suspended catalyst, DPH was completely degraded in both media at pH 6-8, outperforming the EF process with Fe2+ catalyst at pH 3 in terms of degradation rate and mineralization degree thanks to the absence of refractory Fe(III)-carboxylate complexes that typically decelerate the TOC abatement. From the by-products detected by GC/MS, a reaction sequence for DPH mineralization is proposed.


Asunto(s)
Cobre , Peróxido de Hidrógeno , Hierro , Contaminantes Químicos del Agua , Catálisis , Cobre/química , Concentración de Iones de Hidrógeno , Peróxido de Hidrógeno/química , Hierro/química , Contaminantes Químicos del Agua/química , Carbono/química , Estructuras Metalorgánicas/química , Aguas Residuales/química , Difenhidramina/química , Oxidación-Reducción , Residuos de Medicamentos/química
17.
J Environ Health Sci Eng ; 22(1): 313-327, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38887776

RESUMEN

This study applied an electro-Fenton process using chemically modified activated carbon derived from rubber seed shells loaded with α-FeOOH (RSCF) as catalyst to remove tetracycline residues from aquatic environment. Catalyst characteristics were evaluated using SEM, EDS, XRD, and XPS, showing successful insertion of iron onto the activated carbon. The effects of the parameters were investigated, and the highest treatment efficiency was achieved at pH of 3, Fe: H2O2 ratio (w/w) of 500:1, catalyst dose of 1 g/L, initial TCH concentration of 100 mg/L, and electric current of 150 mA, with more than 90% of TCH being eliminated within 30 min. Furthermore, even after five cycles of use, the treatment efficiency remains above 90%. The rate constant is calculated to be 0.218 min-1, with high regression coefficients (R 2 = 0.93). The activation energy (Ea) was found to be 32.2 kJ/mol, indicating that the degradation of TCH was a simple reaction with a low activation energy. These findings showed that the RSCF is a highly efficient and cost-effective catalyst for TCH degradation. Moreover, the use of e-Fenton process has the advantage of high efficiency, low cost thanks to the recyclability of the catalyst, and environmental friendliness thanks to less use of H2O2.

18.
Water Res ; 246: 120674, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37857008

RESUMEN

Electrified membrane technologies have recently demonstrated high potential in tackling water pollution, yet their practical applications are challenged by relying on large precursor doses. Here, we developed a Janus porous membrane (JPEM) with synergic direct oxidation by Magnéli phase Ti4O7 anode and electro-Fenton reactions by CuFe2O4 cathode. Organic pollutants were first directly oxidized on the Ti4O7 anode, where the extracted electrons from pollutants were transported to the cathode for electro-Fenton production of hydroxyl radical (·OH). The cathodic ·OH further enhanced the mineralization of organic pollutant degradation intermediates. With the sequential anodic and cathodic oxidation processes, the reagent-free JPEM showed competitive performance in rapid degradation (removal rate of 0.417 mg L-1 s-1) and mineralization (68.7 % decrease in TOC) of sulfamethoxazole. The JPEM system displayed general performance to remove phenol, carbamazepine, and perfluorooctanoic acid. The JPEM runs solely on electricity and oxygen that is comparable to that of PEM relies on large precursor doses and, therefore, operation friendly and environmental sustainability. The high pollutant removal and mineralization achieved by rational design of the reaction processes sheds light on a new approach for constructing an efficient electrified membrane.


Asunto(s)
Contaminantes Ambientales , Contaminantes Químicos del Agua , Fenol , Fenoles , Electrodos , Oxidación-Reducción , Peróxido de Hidrógeno
19.
Environ Technol ; 44(28): 4334-4351, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-35712767

RESUMEN

The aim of the current study is to investigate the efficacy of the electro-Fenton process in the degradation of favipiravir drugs from aqueous solutions, which has increased in use as a result of the COVID-19 pandemic. The Response Surface Methodology (RSM) was developed using a Central Composite Design (CCD) in which five independent variables, including Fe2+ concentration, current density, initial FVP concentration, pH, and reaction time, were coded with high and low levels, and the maximum removal percentage of FVP (97.8%) and COD (91.65%) were determined as responses. In the EF process, 530 mg/L H2O2 was produced in-situ by cathodic reduction of O2 in aqueous solution and thus FVP has been successfully oxidized through hydroxyl radicals. The H2O2/Fe2+ ratio was determined to be 0.51 under optimum conditions. At the end of the experiment, the maximum energy consumption was found to be 2.12 kWh per g COD. The FVP was completely mineralized in a very short time by the EF process, according to the LC-MS/MS examination. The EF process followed the pseudo first-order kinetic model with the rate constants of 0.023, 0.016 and 0.006 1/min for pH 2, 3 and 4, respectively. According to the findings of this study, the electro-Fenton process is an effective method for removing FVP from aqueous solutions. To the authors' knowledge, this is the first study to show the degradation and optimum conditions of FVP in aqueous solution using the electro-Fenton (EF) process.


Asunto(s)
COVID-19 , Contaminantes Químicos del Agua , Humanos , Aguas Residuales , Peróxido de Hidrógeno , Antivirales , Cromatografía Liquida , Pandemias , Oxidación-Reducción , Espectrometría de Masas en Tándem
20.
Environ Sci Pollut Res Int ; 30(14): 39431-39450, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36763272

RESUMEN

Over the last decades, advanced oxidation processes (AOPs) have been widely used in surface and ground water pollution control. The heterogeneous electro-Fenton (EF) process has gained much attention due to its properties of high catalytic performance, no generation of iron sludge, and good recyclability of catalyst. As of October 2022, the cited papers and publications of EF are around 1.3 × 10-5 and 3.4 × 10-3 in web of science. Among the AOP techniques, the contaminant removal efficiencies by EF process are above 90% in most studies. Current reviews mainly focused on the mechanism of EF and few reviews comprehensively summarized heterogeneous catalysts and their applications in wastewater treatment. Thus, this review focuses on the current studies covering the period 2012-2022, and applications of heterogeneous catalysts in EF process. Two kinds of typical heterogeneous EF systems (the addition of solid catalysts and the functionalized cathode catalysts) and their applications for organic contaminants degradation in water are reviewed. In detail, solid catalysts, including iron minerals, iron oxide-based composites, and iron-free catalysts, are systematically described. Different functionalized cathode materials, containing Fe-based cathodes, carbonaceous-based cathodes, and heteroatom-doped cathodes, are also reviewed. Finally, emphasis and outlook are made on the future prospects and challenges of heterogeneous EF catalyst for wastewater treatments.


Asunto(s)
Contaminantes Químicos del Agua , Agua , Aguas del Alcantarillado , Minerales , Catálisis , Peróxido de Hidrógeno , Contaminantes Químicos del Agua/análisis , Oxidación-Reducción
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