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1.
FEBS Lett ; 594(19): 3122-3141, 2020 10.
Artículo en Inglés | MEDLINE | ID: mdl-32677084

RESUMEN

Target of rapamycin (TOR) kinase is a sensor and a central integrator of internal and external metabolic cues. However, in algae and in higher plants, the components of TOR kinase signaling are yet to be characterized. Here, we establish an assay system to study TOR kinase activity in Chlamydomonas reinhardtii using the phosphorylation status of its putative downstream target, CrS6K. Using this assay, we probe the modulation of cellular TOR kinase activity under various physiological states such as photoautotrophy, heterotrophy, mixotrophy, and nitrogen (N) starvation. Importantly, we uncover that excess acetate in the medium leads to high cellular reactive oxygen species levels, triggering autophagy and a concomitant drop in TOR kinase activity in a dose-dependent manner, thus leading to a N-starvation-like cellular phenotype, even when nitrogen is present.


Asunto(s)
Chlamydomonas reinhardtii/enzimología , Chlamydomonas reinhardtii/metabolismo , Estrés Fisiológico , Serina-Treonina Quinasas TOR/metabolismo , Acetatos/metabolismo , Atrazina/farmacología , Atrazina/efectos de la radiación , Autofagia/efectos de los fármacos , Autofagia/efectos de la radiación , Chlamydomonas reinhardtii/efectos de los fármacos , Chlamydomonas reinhardtii/efectos de la radiación , Procesos Heterotróficos/efectos de los fármacos , Procesos Heterotróficos/efectos de la radiación , Luz , Modelos Biológicos , Mutagénesis Insercional/genética , Procesos Fototróficos/efectos de los fármacos , Procesos Fototróficos/efectos de la radiación , Especies Reactivas de Oxígeno/metabolismo , Reproducibilidad de los Resultados , Transducción de Señal/efectos de los fármacos , Transducción de Señal/efectos de la radiación , Estrés Fisiológico/efectos de los fármacos , Estrés Fisiológico/efectos de la radiación
2.
Environ Sci Pollut Res Int ; 26(23): 23268-23278, 2019 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-31197664

RESUMEN

Four techniques, UV254 nm photolysis, vacuum ultraviolet (VUV172 nm) photolysis, combined UV254 nm/VUV185 nm photolysis and gamma (γ) radiolysis were used to induce the transformation of atrazine in aqueous solution. The effects of dissolved oxygen (atrazine concentration 1 × 10-4 mol L-1 and 4.6 × 10-7 mol L-1) and matrix (high purity water/purified wastewater, atrazine concentration 4.6 × 10-7 mol L-1) and the electric energy requirements were investigated. The calculation of the energy input in cases of the photolyses was based on the lamp's power. In radiolysis, the absorbed dose (J kg-1) was the basis. In UV photolysis, atrazine transforms to atrazine-2-hydroxy; this product practically does not degrade during UV photolysis; due to this reason, the mineralisation is very slow. This and some other products of atrazine decomposition degrade only in radical reactions. Dissolved oxygen usually slightly enhances the degradation rate. At 10-7 mol L-1 concentration level, the matrix, high purity water/purified wastewater, has not much influence on the degradation rates in UV photolysis and radiolysis. In the VUV and UV/VUV systems, considerable matrix effects were observed. Comparing the electric energy requirements of the four degradation processes, radiolysis was found to be the economically most feasible method, requiring 1-2 orders of magnitude less electric energy than UV/VUV, VUV and UV photolysis.


Asunto(s)
Atrazina/análisis , Rayos gamma , Fotólisis , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Atrazina/efectos de la radiación , Cinética , Oxidación-Reducción , Vacio , Aguas Residuales/química , Contaminantes Químicos del Agua/efectos de la radiación
3.
Chemosphere ; 217: 833-842, 2019 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-30453277

RESUMEN

The photocatalytic degradation of atrazine by activated carbon/graphitic carbon nitride composites with peroxymonosulfate (PMS) was investigated under visible light irradiation. The photocatalysts were prepared at different activated carbon (AC) loaded percentages and characterized by XRD, FT-IR, BET surface area, SEM, UV-Vis absorbance, photocurrent response and EIS. Several parameters which might influence the degradation efficiency were studied including PMS concentration, solution pH, catalyst dosage, initial atrazine concentration as well as water matrix effect. The results indicated that incorporation of AC contributes effectively in suppressing the recombination of electron-holes pairs and enhancing the photocatalytic performance of graphitic carbon nitride. More significantly, the degradation efficiency of atrazine showed remarkable improvement with PMS addition under visible light irradiation. The reaction rate constant of the 10% AC/g-C3N4/Vis/PMS system (0.0376 min-1) was approximately 2.9 times higher than that of g-C3N4/Vis/PMS system (0.0128 min-1). Results from quenching tests revealed that both sulfate and hydroxyl radicals were involved in the degradation of atrazine, while the latter is the main contributor. This paper constitutes an insight for the metal-free catalyst activation of PMS by photocatalysis for environmental remediation.


Asunto(s)
Atrazina/química , Luz , Nitrilos/química , Peróxidos/química , Fotólisis , Atrazina/efectos de la radiación , Catálisis , Carbón Orgánico , Restauración y Remediación Ambiental , Grafito/química , Análisis Espectral
4.
Ecotoxicol Environ Saf ; 169: 169-177, 2019 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-30447517

RESUMEN

This study is the first to reveal that the iron-catalyzed photo-activation of persulfate (UV/PS/Fe2+system) under mercury-free KrCl excilamp irradiation (222 nm) is capable of simultaneous degradation of an organic pollutant and inactivation of a microorganism in aqueous media using the herbicide atrazine (ATZ) and E. coli as model contaminants, respectively. Deionized water, natural water and wastewater effluents, contaminated with 4 mg/L ATZ and/or 105 CFU/mL E. coli, were sequentially treated by direct UV, UV/PS and UV/PS/Fe2+ processes. Lowering the pH to 3.5 accelerated both the degradation and inactivation during the UV/PS/Fe2+ treatment of natural water. Comparison of the apparent UV dose-based pseudo first-order rate constants showed the negative effect of E. coli on ATZ degradation by decreasing rates in all of the examined water matrices. This can be due to the competitive effect between ATZ and bacterial cells for reactive oxygen species (ROS). By contrast, E. coli in the presence of ATZ was inactivated faster in natural water and wastewater (but not in deionized water), as compared to the case without ATZ. A scheme of possible synergistic inactivation under ROS exposure in water, containing ATZ, natural organic matter and chloride ions as primary constituents, was proposed. Radical scavenging experiments showed a major contribution of SO4•- to ATZ degradation by UV/PS/Fe2+ treatment of deionized water and natural water. The UV doses, required for 90% removal of ATZ from natural water and wastewater, achieve 160 mJ/cm2 (pH 5.5) and concurrently provide 99.99% E. coli inactivation. These results make the UV/PS/Fe2+ system with narrow band UV light sources promising for simultaneous water treatment and disinfection.


Asunto(s)
Atrazina/análisis , Desinfección/métodos , Escherichia coli/efectos de los fármacos , Compuestos Ferrosos/química , Compuestos de Potasio/química , Sulfatos/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Atrazina/efectos de la radiación , Desinfección/instrumentación , Escherichia coli/efectos de la radiación , Oxidación-Reducción , Aguas Residuales/química , Contaminantes Químicos del Agua/efectos de la radiación , Purificación del Agua/instrumentación
5.
Ecotoxicol Environ Saf ; 163: 620-628, 2018 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-30096663

RESUMEN

Nanosized BaFe1-xCuxO3 powders were prepared using the Pechini method. To limit grain growth and agglomeration, the temperature of calcination was limited to 800 °C. For all samples, the cubic form of BaFeO2.75 was predominant with minor additional phases. Cu doping was found to have a remarkable effect on the structural cubic unit cell parameter as the Cu concentration increased. As shown by XRD,the samples were in the nanometer size range (17-63 nm). However, as the Cu concentration increases, the agglomeration increases with the highest surface area for the BaFe0.95Cu0.05O3 composition, which also displays the highest photocatalytic atrazine degradation. For this sample, more than 90% degradation of atrazine was obtained at the optimum conditions (120 min irradiation under visible light at pH 11 using 0.75 mg of the catalyst). The Atrazine degradation was found to follow the pseudo-order kinetics. GC/MS was used to detect the intermediates and the reaction pathways. All the prepared samples and produced waters at the end of the experiment were found to be nontoxic.


Asunto(s)
Atrazina/efectos de la radiación , Herbicidas/efectos de la radiación , Luz , Óxidos/química , Atrazina/química , Catálisis , Herbicidas/química , Cinética , Óxidos/efectos de la radiación , Fotólisis , Temperatura
6.
Environ Sci Pollut Res Int ; 25(3): 2691-2701, 2018 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-29134527

RESUMEN

In this study, a UV/O3 hybrid advanced oxidation system was used to remove chemical oxygen demand (COD), ammonia nitrogen (NH3-N), and atrazine (ATZ) from ATZ production wastewater. The removal of COD and NH3-N, under different UV and O3 conditions, was found to follow pseudo-first-order kinetics with rate constants ranging from 0.0001-0.0048 and 0.0015-0.0056 min-1, respectively. The removal efficiency of ATZ was over 95% after 180 min treatment, regardless the level of UV power. A kinetic model was further proposed to simulate the removal processes and to quantify the individual roles and contributions of photolysis, direct O3 oxidation, and hydroxyl radical (OH·) induced oxidation. The experimental and kinetic modeling results agreed reasonably well with deviations of 12.2 and 13.1% for the removal of COD and NH3-N, respectively. Photolysis contributed appreciably to the degradation of ATZ, while OH· played a dominant role for the removal of both COD and NH3-N, especially in alkaline environments. This study provides insights into the treatment of ATZ containing wastewater using UV/O3 and broadens the knowledge of kinetics of ozone-based advanced oxidation processes.


Asunto(s)
Atrazina/análisis , Ozono/química , Rayos Ultravioleta , Aguas Residuales/química , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Amoníaco/análisis , Atrazina/efectos de la radiación , Análisis de la Demanda Biológica de Oxígeno , Cinética , Modelos Teóricos , Nitrógeno/análisis , Oxidación-Reducción , Contaminantes Químicos del Agua/efectos de la radiación
7.
Artículo en Inglés | MEDLINE | ID: mdl-28448750

RESUMEN

This work evaluated the feasibility of a photo-Fenton-like process using persulfate (PS) and ferrous iron (Fe2+) under simulated solar radiation for degrading the herbicide atrazine (ATZ, 6-Chloro-N-ethyl-N'-isopropyl-1,3,5-triazine-2,4-diamine) and inactivating E. coli. Milli Q water, lake water, and diluted wastewater effluents were spiked both simultaneously and separately with ATZ (4 mg/L) and E. coli (105 CFU/mL), and exposed to treatment. A method for determining the average irradiance throughout the water media in the UV(A+B) range of the Xe lamp emission was developed for bench-scale experiments. These values were used to calculate the UV(A+B) fluences and the solar UV(A+B) energy doses per unit of volume (QUV(A+B), kJ/L). The obtained kinetic data were presented versus energy dose. Treatment of lake water at near-neutral pH was ineffective via the photo-Fenton-like process, attaining only 20% ATZ removal and 1-log reduction of E. coli. In Milli Q water and wastewater, the complete degradation of ATZ in the absence of bacteria was observed at an average energy dose of 1.5 kJ/L (60 min), while in the presence of cells the degradation efficiency was ∼60%. When ATZ was present, E. coli inactivation was also affected in Milli Q water, with 1.4-log reduction (93%) at a dose of 1.6 kJ/L (60 min), whereas in wastewater complete inactivation was achieved at a lower dose of 1.3 kJ/L (45 min). The energy requirements on a QUV(A+B) basis for simultaneous 90% ATZ removal and 99.99% E. coli inactivation in Milli Q water and wastewater were shown to be less than 10 kJ/L. This suggests the solar/PS/Fe2+ system is promising for simultaneous treatment and disinfection of wastewater effluents.


Asunto(s)
Atrazina/análisis , Escherichia coli/efectos de los fármacos , Peróxido de Hidrógeno/química , Hierro/química , Compuestos de Potasio/química , Sulfatos/química , Luz Solar , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Atrazina/efectos de la radiación , Desinfección/métodos , Escherichia coli/efectos de la radiación , Estudios de Factibilidad , Concentración de Iones de Hidrógeno , Aguas Residuales/química , Aguas Residuales/microbiología , Contaminantes Químicos del Agua/efectos de la radiación
8.
Water Sci Technol ; 75(5-6): 1128-1137, 2017 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-28272041

RESUMEN

Simply coating 1 wt.% of platinum on titanium dioxide (TiO2) surface resulted in simple preparation of platinized TiO2 (Pt-TiO2). This study demonstrated the photodegradation of atrazine (ATZ) using either Pt-TiO2 or TiO2 as a photocatalyst under 352 nm light irradiation. The Pt-TiO2-catalyzed ATZ degradation reached 76% in 3 hours without adding H2O2 solution or aeration, which was more than 10% higher than the TiO2-catalyzed reaction. The decomposition product of Pt-TiO2-catalyzed ATZ degradation was mainly cyanuric acid. Thus, Pt-TiO2 as an effective photocatalyst has three main advantages in the photodegradation of ATZ under 352 nm irradiation. First, the coated Pt can facilitate the generation of appropriate amounts of OH radicals, so it can prevent the formation of over-oxidized TiO2. Second, aeration was not needed. Third, the excited electrons were mainly uni-directionally transferred to the catalyst surface to avoid recombination of electron-hole pairs.


Asunto(s)
Atrazina/efectos de la radiación , Fotólisis , Platino (Metal)/química , Titanio/efectos de la radiación , Atrazina/química , Catálisis/efectos de la radiación , Peróxido de Hidrógeno/química , Cinética , Microscopía Electrónica de Transmisión , Oxidación-Reducción , Espectrofotometría Ultravioleta , Triazinas/química , Difracción de Rayos X
9.
Ecotoxicol Environ Saf ; 137: 35-41, 2017 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-27907844

RESUMEN

The oxidation of s-triazines (using atrazine (ATZ) as a model compound) by a solar-enhanced Fenton-like process involving persulfate and ferrous ion was studied. A flow-through tubular photoreactor was employed for the experiments. The solar-enhanced oxidative system involving ferrous ion and persulfate (Solar/S2O82-/Fe2+) showed the highest ATZ degradation efficiency when compared with other treatments (unactivated S2O82-, Solar - sunlight only, S2O82-/Fe2+, Solar/S2O82-). Complete degradation of ATZ and 20% reduction in total organic carbon (TOC) content were observed after 30min of the treatment. The in situ generated •ОН and SO4-• radicals were shown to be involved in ATZ oxidation using the radical scavengers methanol and tert-butyl alcohol. Furthermore, iron compounds were shown to act not only as catalysts but also as photo-sensitizers, as the introduction of ferrous ion into the reaction mixture led to an increased absorbance of the solution and expansion of the absorption spectrum into the longer wavelength spectral region.


Asunto(s)
Atrazina/análisis , Compuestos Ferrosos/química , Peróxido de Hidrógeno/química , Hierro/química , Sulfatos/química , Luz Solar , Contaminantes Químicos del Agua/análisis , Atrazina/química , Atrazina/efectos de la radiación , Modelos Teóricos , Oxidación-Reducción , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/efectos de la radiación
10.
Chemosphere ; 157: 79-88, 2016 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-27209556

RESUMEN

The present study investigates the efficiency of a sustainable treatment technology, the electrophotocatalytic (EPC) process using innovative photoanode TiO2-x prepared by a magnetron sputter deposition process to remove the herbicide atrazine (ATZ) from water. The coexistence of anatase and rutile were identified by X-ray diffraction (XRD) and the presence of oxygen vacancies reduce the value of the observed bandgap to 3.0 eV compared to the typical 3.2 eV TiO2, this reduction is concomitant with a partial phase transition which is probably responsible for the increase in photoactivity. The experimental results with an initial concentration of ATZ (100 µg L(-1)) show that more than 99% of ATZ oxidation was obtained after 30 min of treatment and reaction kinetic constant was about 0.146 min(-1). This good efficiency indicates that EPC process is an efficient, simple and green technique for degradation of pesticides such as ATZ in water. The analysis with liquid chromatography technique permits to identify, quantify and see the evolution of ATZ by-products which are generated by dechlorination, dealkylation and alkylic-oxidation mechanisms. Finally, the possible pathways of ATZ degradation by hydroxyl radicals were proposed.


Asunto(s)
Atrazina/análisis , Técnicas Electroquímicas/métodos , Titanio/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Atrazina/química , Atrazina/efectos de la radiación , Catálisis , Electrodos , Radical Hidroxilo/química , Cinética , Modelos Teóricos , Oxidación-Reducción , Soluciones , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/efectos de la radiación , Difracción de Rayos X
11.
Water Res ; 92: 78-86, 2016 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-26841231

RESUMEN

Photocatalyst plays a vital role in the photochemical water treatment. To improve the visible-light photoactivity of TiO2 for refractory pollutant degradation, CdS/TiO2 hybrids with different nanostructures have been prepared, but usually suffer from a low photocatalytic degradation efficiency and a rapid photocorrosion. In this work, we developed a synergistic ZnO/CdS/TiO2 hybrid, which could act as a robust and self-protected photocatalyst for water purification without additional sacrificial reagents. This was attributed to the two different junction mechanisms in one single hybrid. Photons were selectively adsorbed by ZnO and CdS, then, the electrons with a low reductive activity in ZnO recombined directly with the holes with a low oxidative activity in CdS, whereas the holes with a high oxidative activity in ZnO and the electrons with a high reductive activity in CdS were captured for catalytic reaction. The superiority of the novel ZnO/CdS/TiO2 hybrid over the traditional CdS/TiO2 hybrid in both photocatalytic activity and anti-photocorrosion capacity was demonstrated in the degradation of Atrazine and Rhodamine B, two typical refractory organic pollutants, and the treatment of real textile wastewater under solar light irradiation. The developed ZnO/CdS/TiO2 hybrid exhibited an excellent potential for the degradation of refractory pollutants, and provided a new way to advance intrinsically solar-susceptible catalyst for photochemical wastewater treatment.


Asunto(s)
Compuestos de Cadmio/química , Sulfuros/química , Luz Solar , Titanio/química , Contaminantes Químicos del Agua/efectos de la radiación , Óxido de Zinc/química , Atrazina/efectos de la radiación , Catálisis/efectos de la radiación , Electricidad , Cinética , Rodaminas/efectos de la radiación , Espectrometría por Rayos X , Textiles , Aguas Residuales/química
12.
J Hazard Mater ; 294: 1-8, 2015 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-25827391

RESUMEN

VUV/UV is a chemical-free and straightforward solution for the degradation of emerging contaminants from water sources. The objective of this work was to investigate the feasibility of VUV/UV advanced oxidation process for the effective degradation of a target micropollutant, atrazine, under continuous flow operation of 0.5-6.5L/min. To provide an in-depth understanding of process, a comprehensive computational fluid dynamics (CFD) model, incorporating flow hydrodynamics, 185nm VUV and 254nm UV radiation propagation along with a complete kinetic scheme, was developed and validated experimentally. The experimental degradation rates and CFD predicted values showed great consistency with less than 2.9% average absolute relative deviation (AARD). Utilizing the verified model, energy-efficiency of the VUV/UV process under a wide range of reactor configurations was assessed in terms of electrical energy-per-order (EEO), OH concentration as well as delivered UV and VUV dose distributions. Thereby, the extent of mixing and circulation zones was found as key parameter controlling the treatment economy and energy-efficiency of the VUV/UV process. Utilizing a CFD-driven baffle design strategy, an improved VUV/UV process with up to 72% reduction in the total electrical energy requirement of atrazine degradation was introduced and verified experimentally.


Asunto(s)
Atrazina/efectos de la radiación , Rayos Ultravioleta , Contaminantes Químicos del Agua/efectos de la radiación , Diseño Asistido por Computadora , Hidrodinámica , Radical Hidroxilo/química , Oxidación-Reducción , Eliminación de Residuos Líquidos/métodos , Contaminación del Agua
13.
J Hazard Mater ; 288: 147-57, 2015 May 15.
Artículo en Inglés | MEDLINE | ID: mdl-25725267

RESUMEN

The degradation of atrazine was investigated in aqueous solution by gamma-ray irradiation. 8.11 µM initial atrazine concentration could be completely removed in N2 saturated solution by applying 3500 Gy radiation dose at a dose rate of 296 Gy h(-1). Significant removal of atrazine (i.e., 39.4%) was observed at an absorbed dose of 1184 Gy in air saturated solution and the removal efficiency was promoted to 50.5 and 65.4% in the presence of N2O and N2 gases, respectively. The relative contributions of hydrated electron, hydroxyl radical and hydrogen radical toward atrazine degradation were determined as ratio of observed dose constant (kobs) and found to be 5: 3: 1 for keaq(-): k·OH: kH·, respectively. The degradation efficiency of atrazine was 69.5, 55.6 and 37.3% at pH 12.1, 1.7 and 5.7, respectively. A degradation mechanism was proposed based on the identified degradation by-products by gas chromatography-mass spectrometry. Taking the relative contributions of oxidative and reductive species to atrazine degradation into account, reductive pathway proved to be a better approach for the radiolytic treatment of atrazine contaminated water.


Asunto(s)
Atrazina/química , Atrazina/efectos de la radiación , Herbicidas/química , Herbicidas/efectos de la radiación , Radical Hidroxilo/química , Protones , Cromatografía de Gases y Espectrometría de Masas , Concentración de Iones de Hidrógeno , Cinética , Eliminación de Residuos Líquidos , Contaminantes Químicos del Agua , Purificación del Agua , Rayos X
14.
J Hazard Mater ; 275: 166-74, 2014 Jun 30.
Artículo en Inglés | MEDLINE | ID: mdl-24862347

RESUMEN

The effectiveness of sonolysis (US), photolysis (UV), and sonophotolysis (USUV) for the degradation of atrazine (ATZ) was investigated. An untypical kinetics analysis was found useful to describe the combined process, which is compatible to pseudo first-order kinetics. The heterogeneous environments of two different ultrasounds (20 and 400 kHz) were evaluated. The heterogeneous distribution of ATZ in the ultrasonic solution was found critical in determining the reaction rates at different frequencies. The presence of NaCl would promote/inhibit the rates by the growth and decline of "salting out" effect and surface tension. The benefits of combining these two processes were for the first time investigated from the aspect of promoting the intermediates degradation which were resistant in individual processes. UV caused a rapid transformation of ATZ to 2-hydroxyatrazine (OIET), which was insensitive to UV irradiation; however, US and USUV were able to degrade OIET and other intermediates through •OH attack. On the other hand, UV irradiation also could promote radical generation via H2O2 decomposition, thereby resulting in less accumulation of more hydrophilic intermediates, which are difficult to degradation in the US process. Reaction pathways for ATZ degradation by all three processes are proposed. USUV achieved the greatest degree of ATZ mineralization with more than 60% TOC removed, contributed solely by the oxidation of side chains. Ammeline was found to be the only end-product in both US and USUV processes.


Asunto(s)
Atrazina/efectos de la radiación , Herbicidas/efectos de la radiación , Sonicación , Rayos Ultravioleta , Purificación del Agua/métodos , Atrazina/química , Herbicidas/química , Microburbujas , Oxidación-Reducción , Fotólisis , Cloruro de Sodio/química , Triazinas/química
15.
J Environ Sci Health B ; 48(11): 927-34, 2013.
Artículo en Inglés | MEDLINE | ID: mdl-23998304

RESUMEN

The degradation of atrazine in aqueous solution by UV or UV/H2O2 processes, and the toxic effects of the degradation products were explored. The mineralization of atrazine was not observed in the UV irradiation process, resulting in the production of hydroxyatrazine (OIET) as the final product. In the UV/H2O2 process, the final product was ammeline (OAAT), which was obtained by two different pathways of reaction: dechlorination followed by hydroxylation, and the de-alkylation of atrazine. The by-products of the reaction of dechlorination followed by hydroxylation were OIET and hydroxydeethyl atrazine (OIAT), and those of de-alkylation were deisopropyl atrazine (CEAT), deethyl atrazine (CIAT), and deethyldeisopropyl atrazine (CAAT). OIAT and OAAT appeared to be quite stable in the degradation of atrazine by the UV/H2O2 process. In a toxicity test using Daphnia magna, the acute toxic unit (TUa) was less than 1 of TUa (100/EC50, %) in the UV/H2O2 process after 30 min of reaction time, while 1.2 to 1.3 of TUa was observed in the UV process. The TUa values of atrazine and the degradation products have the following decreasing order: OIET> Atrazine> CEAT≈CIAT> CAAT. OIAT and OAAT did not show any toxic effects.


Asunto(s)
Atrazina/química , Atrazina/efectos de la radiación , Herbicidas/química , Herbicidas/efectos de la radiación , Peróxido de Hidrógeno/química , Rayos Ultravioleta , Animales , Cromatografía Liquida , Daphnia/efectos de los fármacos , Espectrometría de Masas , Pruebas de Toxicidad
16.
Environ Technol ; 34(5-8): 1043-51, 2013.
Artículo en Inglés | MEDLINE | ID: mdl-23837356

RESUMEN

The breakdown of pesticides has been promoted by many methods for clean up of contaminated soil and wastewaters. The main goal is to decrease the toxicity of the parent compound to achieve non-toxic compounds or even, when complete mineralization occurs, carbon dioxide and water. Therefore, electrochemical degradation (potentiostatic and galvanostatic) of both the pesticide atrazine and cyanuric acid (CA) at boron-doped diamond (BDD) and Ti/Ru0.3Ti0.7O2 dimensionally stable anode (DSA) electrodes, in different supporting electrolytes (NaCl and Na2SO4), is presented with the aim of establishing the influence of the operational parameters on the process efficiency. The results demonstrate that both the electrode material and the supporting electrolyte have a strong influence on the rate of atrazine removal. In the chloride medium, the rate of atrazine removal is always greater than in sulfate under all conditions employed. Furthermore, in the sulfate medium, atrazine degradation was significant only at the BDD electrode. The total organic carbon (TOC) load decreased by 79% and 56% at the BDD and DSA electrodes, respectively, in the chloride medium. This trend was maintained in the sulfate medium but the TOC removal was lower (i.e. 33% and 13% at BDD and DSA electrodes, respectively). CA, a stable atrazine degradation intermediate, was also studied and it is efficiently removed using the BDD electrode in both media, mainly when high current densities are employed. The use of the BDD electrode in the chloride medium not only degrades atrazine but also mineralized cyanuric acid leading to the higher TOC removal.


Asunto(s)
Atrazina/química , Boro/química , Diamante/química , Electroquímica/instrumentación , Triazinas/química , Contaminantes Químicos del Agua/química , Purificación del Agua/instrumentación , Atrazina/aislamiento & purificación , Atrazina/efectos de la radiación , Electrodos , Diseño de Equipo , Análisis de Falla de Equipo , Herbicidas/química , Herbicidas/aislamiento & purificación , Herbicidas/efectos de la radiación , Óxidos/química , Triazinas/aislamiento & purificación , Triazinas/efectos de la radiación , Contaminantes Químicos del Agua/aislamiento & purificación , Contaminantes Químicos del Agua/efectos de la radiación
17.
Environ Sci Technol ; 47(1): 533-41, 2013 Jan 02.
Artículo en Inglés | MEDLINE | ID: mdl-23215162

RESUMEN

Surface chemistry determines the interactions of sorbate and solvent molecules with the pore wall surfaces of microporous minerals, and affects the transmission and absorption of microwave radiation for a given solvent-sorbate-sorbent system. The sorption and microwave-induced degradation of atrazine in the micropores of nine Y zeolites with different densities (0.16-2.62 site/nm(2)) and types (Mg(2+), Ca(2+), H(+), Na(+), and NH(4)(+)) of surface cations were studied. The influence of the content of cosorbed water in the mineral micropores on atrazine degradation rate was also examined. The results indicate the presence of surface cations at around 0.23 site/nm(2) on the pore wall surface was optimal for atrazine degradation, probably due to formation of insufficient number of "hot spots" with too few cations but excessive competition for microwave energy with too many hydrated cations. Atrazine degraded faster in the presence of cations with lower hydration free energies, which could be attributed to less microwave energy consumption to desorb the bounded water molecules. Reducing the content of coadsorbed water in the micropores also increased atrazine degration rate because of less competition for microwave energy from water. Such mechanistic understanding can guide the design and selection of microporous minerals in the practical application of microwave-induced degradation.


Asunto(s)
Atrazina/química , Herbicidas/química , Microondas , Zeolitas/química , Adsorción , Atrazina/efectos de la radiación , Herbicidas/efectos de la radiación , Porosidad , Propiedades de Superficie
18.
Photochem Photobiol Sci ; 12(4): 660-3, 2013 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-23069861

RESUMEN

Photochemical degradation of atrazine under different conditions was studied and compared, namely degradation via photocatalysis on TiO2, UV C photolysis, and homogeneous photocatalysis in the presence of added ferric ions. The reaction rate constants in heterogeneous photocatalytic reactions on TiO2 and of photolytic degradation by means of UV C light are similar, 0.018 min(-1) and 0.020 min(-1), respectively. The reaction rate constants in homogeneous photocatalytic reactions with Fe(III) added depend strongly on the Fe(III) concentration, 0.0017 min(-1) for 1.6 × 10(-6) mol l(-1) Fe(III) to 0.105 min(-1) for 3.3 × 10(-4) mol l(-1) Fe(III). In all types of reactions, dechlorination was observed; in homogeneous photocatalytic reactions and in UV C (250-300 nm) photolysis, dechlorination proceeds with a 1 : 1 stoichiometry to atrazine degradation, in photocatalytic reactions on TiO2, dechlorination measured as chloride ion release reaches only 1/5 of the substrate degradation. In photocatalytic reactions on TiO2, mineralisation of 40% carbon was observed.


Asunto(s)
Atrazina/química , Herbicidas/química , Rayos Ultravioleta , Atrazina/efectos de la radiación , Catálisis , Cloruros/química , Compuestos Férricos/química , Herbicidas/efectos de la radiación , Fotólisis , Titanio/química
19.
Environ Sci Technol ; 46(9): 5067-76, 2012 May 01.
Artículo en Inglés | MEDLINE | ID: mdl-22489838

RESUMEN

The herbicide atrazine is a common pollutant in reservoirs and other sources of drinking water worldwide. The adsorption of atrazine from water onto zeolites CBV-720 and 4A, mesoporous silica MCM-41, quartz sand, and diatomite, and its microwave-induced degradation when sorbed on these minerals, were studied. Dealuminated HY zeolite CBV-720 exhibited the highest atrazine sorption capacity among the mineral sorbents because of its high micropore volume, suitable pore sizes, and surface hydrophobicity. Atrazine sorbed on the minerals degraded under microwave irradiation due to interfacial selective heating by the microwave, while atrazine in aqueous solution and associated with PTFE powder was not affected. Atrazine degraded rapidly in the micropores of CBV-720 under microwave irradiation and its degradation intermediates also decomposed with further irradiation, suggesting atrazine could be fully mineralized. Two new degradation intermediates of atrazine, 3,5-diamino-1,2,4-triazole and guanidine, were first identified in this study. The evolution of degradation intermediates and changes in infrared spectra of CBV-720 after microwave irradiation consistently indicate the creation of microscale hot spots in the micropores and the degradation of atrazine following a pyrolysis mechanism. These results indicate that microporous mineral sorption coupled with microwave-induced degradation could serve as an efficient treatment technology for removing atrazine from drinking water.


Asunto(s)
Atrazina/efectos de la radiación , Herbicidas/efectos de la radiación , Microondas , Contaminantes Químicos del Agua/efectos de la radiación , Zeolitas/química , Adsorción , Atrazina/química , Herbicidas/química , Espectrofotometría Infrarroja , Contaminantes Químicos del Agua/química
20.
Water Res ; 46(3): 669-78, 2012 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-22153354

RESUMEN

Pulsed light technology consists of a successive repetition of short duration (325µs) and high power flashes emitted by xenon lamps. These flashlamps radiate a broadband emission light (approx. 200-1000 nm) with a considerable amount of light in the short-wave UV spectrum. In the present work, this technology was tested as a new tool for the degradation of the herbicide atrazine in water. To evaluate the presence and evolution with time of this herbicide, as well as the formation of derivatives, liquid chromatography-mass spectrometry (electrospray ionization) ion trap operating in positive mode was used. The degradation process followed first-order kinetics. Fluences about 1.8-2.3 J/cm(2) induced 50% reduction of atrazine concentration independently of its initial concentration in the range 1-1000 µg/L. Remaining concentrations of atrazine, below the current legal limit for pesticides, were achieved in a short period of time. While atrazine was degraded, no chlorinated photoproducts were formed and ten dehalogenated derivatives were detected. The molecular structures for some of these derivatives could be suggested, being hydroxyatrazine the main photoproduct identified. The different formation profiles of photoproducts suggested that the degradation pathway may include several successive and competitive steps, with subsequent degradation processes taking part from the already formed degradation products. According to the degradation efficiency, the short treatment time and the lack of chloroderivatives, this new technology could be considered as an alternative for water treatment.


Asunto(s)
Atrazina/efectos de la radiación , Luz , Fotoquímica/métodos , Fotólisis/efectos de la radiación , Contaminantes Químicos del Agua/efectos de la radiación , Agua/química , Atrazina/química , Cromatografía Liquida , Cinética , Espectrometría de Masas , Espectrofotometría Ultravioleta , Contaminantes Químicos del Agua/química
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