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1.
J Hazard Mater ; 392: 122315, 2020 06 15.
Artículo en Inglés | MEDLINE | ID: mdl-32097853

RESUMEN

This work demonstrates a facile route to assemble MIL-53(Fe) by solvothermal method. Sulfate radical-based advanced oxidation processes (SR-AOPs) coupling with photocatalysis based on MIL-53(Fe) were investigated under visible light. The catalytic effect of MIL-53(Fe) for the degradation of tetracycline hydrochloride (TC-HCl) was systematically studied, as well as the reusability of the catalyst and the effect of operating parameters. The results indicated that 99.7 % of TC (300 mg/L) could be degraded within 80 min in the SR-AOPs coupling with photocatalysis processes, as compared to 71.4 % for the SR-AOPs and only 17.1 % for the photocatalysis. The trapping experiments and electron spin-resonance spectroscopy (ESR) showed the photogenerated electrons of MIL-53(Fe) under visible light irritation were trapped by persulfate to generated sulfate radicals which effectively suppressed the recombination of photogenerated carriers. And also, the SO4- could be formed by the conversion between Fe (Ⅲ) and Fe (Ⅱ) in MIL-53(Fe). Moreover, OH and O2- generated by the reaction increased significantly due to the increase of SO4- which generated more OH and reduced photogenerated carrier recombination respectively. Thus, the degradation efficiency of TC-HCl was improved. Furthermore, the degradation pathway for TC-HCl was proposed using the theoretical calculations and liquid chromatography coupled with mass spectrometry.


Asunto(s)
Antibacterianos/química , Hierro/efectos de la radiación , Luz , Estructuras Metalorgánicas/efectos de la radiación , Compuestos de Sodio/efectos de la radiación , Sulfatos/efectos de la radiación , Tetraciclina/química , Contaminantes Químicos del Agua/química , Catálisis , Hierro/química , Estructuras Metalorgánicas/química , Oxidación-Reducción , Procesos Fotoquímicos , Compuestos de Sodio/química , Sulfatos/química
2.
Ecotoxicol Environ Saf ; 187: 109779, 2020 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-31639643

RESUMEN

UV-activated persulfate (UV/PS) and peroxymonosulfate (UV/PMS) processes as alternative methods for removal of imidacloprid (IMP) were conducted for the first time. The reaction rate constants between IMP and the sulfate or hydroxyl radical were calculated as 2.33×109  or 2.42×1010 M-1 s-1, respectively. The degradation of IMP was greatly improved by UV/PS and UV/PMS compared with only UV or oxidant. At any given dosage, UV/PS achieved higher IMP removal rate than UV/PMS. The pH range affecting the degradation in the UV/PS and UV/PMS systems were different in the ranges of 6-8 and 9 to 10. SO42-, F- and NO3- had no obvious effect on the degradation in the UV/PS and UV/PMS systems. CO32- and PO43- inhibited the degradation of IMP in the UV/PS system, while they enhanced the degradation in the UV/PMS system. Algae organic matters (AOM) were used to consider the impact of the degradation of IMP for the first time. The removal of IMP were restrained by both AOM and natural organic matters. The higher removal rate of IMP demonstrated that both UV/PS and UV/PMS were suitable for treating the water containing IMP, while UV/PS was cost-effective than UV/PMS based on the total cost calculation. Finally, the degradation pathways of IMP were proposed.


Asunto(s)
Neonicotinoides/análisis , Nitrocompuestos/análisis , Peróxidos/química , Compuestos de Sodio/química , Sulfatos/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Cinética , Modelos Teóricos , Oxidación-Reducción , Peróxidos/efectos de la radiación , Compuestos de Sodio/efectos de la radiación , Sulfatos/efectos de la radiación
3.
Radiat Prot Dosimetry ; 187(2): 164-173, 2019 Dec 31.
Artículo en Inglés | MEDLINE | ID: mdl-31251359

RESUMEN

The thermoluminescence (TL) spectra and dose responses of strontium sulphate doped with rare earth ions show that the SrSO4:Eu2+ phosphor might reasonably be assumed a isoelectronic trap sample which has unique TL characteristics: there is only one obvious glow peak at 385 nm, 489 K in the TL 3D emission spectra and its TL dose response is linear-sublinear. However, there are several elementary glow peaks in the TL 3D emission spectra and their TL dose responses are linear-supralinear for SrSO4:RE3+ (RE = Dy, Tm). These TL peaks occurred from low to high temperature indicate that the traps are distributed in different energy levels. When a suitable amount of other impurities co-doped into these SrSO4:RE3+, such as phosphorus, the relative intensities of these elementary glow peaks are changed significantly, especially the TL peak ~500 K is enhanced while the peaks at lower temperature are suppressed. The enhanced peak of SrSO4:RE3+,P is attributed to the deep traps. Their dose responses remain in nonlinearity when co-doped phosphorus. The above results and the luminescence properties of other sulphate doped rare earths impurities illustrate that the TL characteristics depend on the structure of defect complexes which can be assumed the basic elements in the TL multi-stage processes.


Asunto(s)
Mediciones Luminiscentes/métodos , Metales de Tierras Raras/química , Fósforo/química , Estroncio/efectos de la radiación , Sulfatos/efectos de la radiación , Dosimetría Termoluminiscente/métodos , Disprosio/química , Europio/química , Luminiscencia , Estroncio/química , Sulfatos/química
4.
Water Res ; 133: 299-309, 2018 04 15.
Artículo en Inglés | MEDLINE | ID: mdl-29407711

RESUMEN

The widespread occurrence of pharmaceuticals and their metabolites in natural waters has raised great concerns about their potential risks on human health and ecological systems. This study systematically investigates the degradation of sulfasalazine (SSZ) and its two human metabolites, sulfapyridine (SPD) and 5-aminosalicylic acid (5-ASA), by UV and UV/peroxydisulfate (UV/PDS) processes. Experimental results show that SPD and 5-ASA were readily degraded upon UV 254 nm direct photolysis, with quantum yields measured to be (8.6 ±â€¯0.8) × 10-3 and (2.4 ±â€¯0.1) × 10-2 mol Einstein-1, respectively. Although SSZ was resistant to direct UV photolysis, it could be effectively removed by both UV/H2O2 and UV/PDS processes, with fluence-based pseudo-first-order rate constants determined to be 0.0030 and 0.0038 cm2 mJ-1, respectively. Second-order rate constant between SO4•- and SSZ was measured as (1.33 ±â€¯0.01) × 109 M-1s-1 by competition kinetic method. A kinetic model was established for predicting the degradation rate of SSZ in the UV/PDS process. Increasing the dosage of PDS significantly enhanced the degradation of SSZ in the UV/PDS process, which can be well predicted by the developed kinetic model. Natural water constituents, such as natural organic matter (NOM) and bicarbonate (HCO3-), influenced the degradation of SSZ differently. The azo functional group of SSZ molecule was predicted as the reactive site susceptible to electrophilic attack by SO4•- by frontier electron densities (FEDs) calculations. Four intermediate products arising from azo bond cleavage and SO2 extrusion were identified by solid phase extraction-liquid chromatography-triple quadrupole mass spectrometry (SPE-LC-MS/MS). Based on the products identified, detailed transformation pathways for SSZ degradation in the UV/PDS system were proposed. Results reveal that UV/PDS could be an efficient approach for remediation of water contaminated by SSZ and its metabolites.


Asunto(s)
Compuestos de Sodio/efectos de la radiación , Sulfasalazina/química , Sulfasalazina/efectos de la radiación , Sulfatos/efectos de la radiación , Rayos Ultravioleta , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/efectos de la radiación , Humanos , Peróxido de Hidrógeno/química , Peróxido de Hidrógeno/efectos de la radiación , Cinética , Mesalamina/química , Mesalamina/efectos de la radiación , Oxidación-Reducción , Fotólisis , Compuestos de Sodio/química , Sulfapiridina/química , Sulfapiridina/efectos de la radiación , Sulfatos/química , Purificación del Agua
5.
Water Res ; 132: 190-199, 2018 04 01.
Artículo en Inglés | MEDLINE | ID: mdl-29331907

RESUMEN

Membrane fouling is a recognized obstacle for the application of ultrafiltration (UF) for drinking water treatment. In this study, ultraviolet/persulfate (UV/PS) oxidation was employed as a pretreatment to control membrane fouling caused by natural organic matter (NOM) in surface water. The effects of UV/PS pretreatment on amounts and characteristics of NOM were investigated in terms of dissolved organic carbon, fluorescent spectrum, molecular weight distribution and hydrophobicity. UF membrane fouling during filtration of raw and pre-oxidized water was compared with transmembrane pressure development, and the fouled membranes were further characterized using scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FTIR). The results indicate that NOM was considerably degraded and partially mineralized (∼58%) by UV/PS pretreatment at a PS dose not exceeding 0.6 mM and a UV irradiation time within 120 min, which was attributed to the generation of sulfate and hydroxyl radicals. The fluorescent compounds in NOM were almost completely degraded (>98%) by the UV/PS pretreatment at a PS dose of 0.4 mM, except for tyrosine-like proteins (∼80%). Moreover, UV/PS pretreatment decreased the ratio of macromolecular compounds and increased the hydrophilic fractions, resulting in reduced NOM adhesion to the membrane. Hence, irreversible fouling by NOM was significantly retarded (∼75%) by the UV/PS pretreatment due to reduction in NOM, and more importantly by preferential degradation of fluorescent, macromolecular and hydrophobic compounds. Fouling control performance was considerably improved at increased PS doses and extended UV irradiation time.


Asunto(s)
Compuestos de Sodio/química , Compuestos de Sodio/efectos de la radiación , Sulfatos/química , Sulfatos/efectos de la radiación , Rayos Ultravioleta , Contaminantes del Agua/química , Purificación del Agua/métodos , Interacciones Hidrofóbicas e Hidrofílicas , Membranas Artificiales , Peso Molecular , Oxidación-Reducción , Ultrafiltración/instrumentación , Ultrafiltración/métodos , Purificación del Agua/instrumentación
6.
Ecotoxicol Environ Saf ; 141: 139-147, 2017 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-28340369

RESUMEN

Diclofenac (DCF) is the frequently detected non-steroidal pharmaceuticals in the aquatic environment. In this study, the degradation of DCF was evaluated by UV-254nm activated persulfate (UV/PS). The degradation of DCF followed the pseudo first-order kinetics pattern. The degradation rate constant (kobs) was accelerated by UV/PS compared to UV alone and PS alone. Increasing the initial PS dosage or solution pH significantly enhanced the degradation efficiency. Presence of various natural water constituents had different effects on DCF degradation, with an enhancement or inhibition in the presence of inorganic anions (HCO3- or Cl-) and a significant inhibition in the presence of NOM. In addition, preliminary degradation mechanisms and major products were elucidated using LC-MS/MS. Hydroxylation, decarbonylation, ring-opening and cyclation reaction involving the attack of SO4•- or other substances, were the main degradation mechanism. TOC analyzer and Microtox bioassay were employed to evaluate the mineralization and cytotoxicity of solutions treated by UV/PS at different times, respectively. Limited elimination of TOC (32%) was observed during the mineralization of DCF. More toxic degradation products and their related intermediate species were formed, and the UV/PS process was suitable for removing the toxicity. Of note, longer degradation time may be considered for the final toxicity removal.


Asunto(s)
Diclofenaco/análisis , Sulfatos/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/análisis , Purificación del Agua/métodos , Cromatografía Liquida , Diclofenaco/química , Diclofenaco/toxicidad , Cinética , Oxidación-Reducción , Sulfatos/efectos de la radiación , Espectrometría de Masas en Tándem , Vibrio/efectos de los fármacos , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/toxicidad
7.
Water Sci Technol ; 2017(1): 126-133, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-29698228

RESUMEN

Antibiotics are known today as emerging contaminants due to potentially adverse effects on aquatic ecosystems and the health of humans and animals, even at very low concentrations. The present study was conducted to evaluate the efficiency of the UV/S2O8 process and affecting factors (pH, initial metronidazole (MNZ) concentration, initial persulfate concentration and reaction time) in removing antibiotic MNZ. The results obtained from the experiments showed that the UV/S2O8 process efficiency is higher in acidic pH values due to production of further radical SO4- and increases with extended contact time, but the efficiency of the process is reduced by increasing the concentration of MNZ. In assessing the effect of initial persulfate concentration on the process efficiency, MNZ removal efficiency was also increased by 99.5% after contact time of 35 min with increasing the initial persulfate concentration up to 1 g/L. However, the process efficiency was decreased at higher concentrations (2 mg/L) due to reaction of sulfate radicals with each other or with persulfate and its saturation. The kinetic data fitted the pseudo-first-order kinetic model (R2 > 99%). The findings of this study clearly demonstrated the high potential of the UV/S2O8 process in the degradation of MNZ.


Asunto(s)
Metronidazol/química , Contaminantes Químicos del Agua/química , Purificación del Agua/métodos , Antiinfecciosos/química , Cinética , Oxidación-Reducción , Procesos Fotoquímicos , Sulfatos/efectos de la radiación , Rayos Ultravioleta
8.
J Environ Manage ; 166: 12-22, 2016 Jan 15.
Artículo en Inglés | MEDLINE | ID: mdl-26468603

RESUMEN

The removal of Bisphenol-A (BPA) from contaminated water using advanced oxidation methods such as UV-C assisted oxidation by hydrogen peroxide (H2O2) and sodium persulfate (SPS) has been reported by the authors earlier (Sharma et al., 2015a). In the present study, the authors report the removal of BPA from aqueous solution by the above two methods and its degradation mechanism. UV-C light (254 nm wavelength, 40 W power) was applied to BPA contaminated water at natural pH (pHN) under room temperature conditions. Experiments were carried out with the initial BPA concentration in the range of 0.04 mM-0.31 mM and the oxidant/BPA molar ratio in the range of 294:1-38:1 for UV-C/H2O2 and 31.5-4.06:1 for UV-C/SPS systems. The removal of BPA enhanced with decreasing BPA concentration. The total organic carbon also decreased with the UV-C irradiation time under optimum conditions ([H2O2]0 = 11.76 mM; [SPS]0 = 1.26 mM; temperature (29 ± 3 °C). Competition of BPA for reaction with HO or [Formula: see text] radicals at its higher concentrations results in a decrease in the removal of BPA. The intermediates with smaller and higher molecular weights than that of BPA were found in the treated water. Based on GC-MS and FTIR spectra of the reaction mixture, the formation of hydroxylated by-products testified the HO mediated oxidation pathway in the BPA degradation, while the formation of quinones and phenoxy phenols pointed to the [Formula: see text] dominating pathway through the formation of hydroxycyclohexadienyl (HCHD) and BPA phenoxyl radicals. The main route of BPA degradation is the hydroxylation followed by dehydration, coupling and ring opening reactions.


Asunto(s)
Compuestos de Bencidrilo/química , Peróxido de Hidrógeno/química , Fenoles/química , Compuestos de Sodio/química , Sulfatos/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/química , Purificación del Agua/métodos , Compuestos de Bencidrilo/análisis , Radicales Libres/química , Radicales Libres/efectos de la radiación , Cromatografía de Gases y Espectrometría de Masas , Peróxido de Hidrógeno/efectos de la radiación , Oxidantes , Oxidación-Reducción , Fenoles/análisis , Compuestos de Sodio/efectos de la radiación , Sulfatos/efectos de la radiación , Contaminantes Químicos del Agua/análisis
9.
J Hazard Mater ; 305: 229-239, 2016 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-26686482

RESUMEN

Oxytetracycline (OTC), an important broad-spectrum antibiotic, has been detected extensively in various environmental systems, which may have a detrimental impact on ecosystem and human health through the development of drug resistant bacteria and pathogens. In this study, the degradation of OTC was evaluated by UV-254nm activated persulfate (PS). The observed UV fluence based pseudo first-order rate constant (kobs) was found to be the highest at near neutral pH conditions (pH 5.5-8.5). Presence of various natural water constituents had different effects on OTC degradation, with a significant enhancement in the presence of bicarbonate or Cu(2+). Limited elimination of total organic carbon (TOC) and PS was observed during the mineralization of OTC. Transformation byproducts in the presence and absence of hydroxyl radical scavenging agent tert-butanol (t-BuOH) were identified using ultra-high definition accurate-mass quadrupole time-of-flight liquid chromatography/mass spectrometer (LC-QTOF/MS). Potential OTC degradation mechanism was subsequently proposed revealing four different reaction pathways by SO4(-) reaction including hydroxylation (+16Da), demethylation (-14Da), decarbonylation (-28Da) and dehydration (-18Da). This study suggests that UV-254nm/PS is a promising treatment technology for the control of water pollution caused by emerging contaminants such as OTC.


Asunto(s)
Antibacterianos/química , Oxitetraciclina/química , Compuestos de Sodio/química , Compuestos de Sodio/efectos de la radiación , Sulfatos/química , Sulfatos/efectos de la radiación , Rayos Ultravioleta , Contaminantes Químicos del Agua/química , Cinética , Purificación del Agua/métodos
10.
Environ Sci Pollut Res Int ; 23(3): 2848-55, 2016 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-26452660

RESUMEN

The degradation kinetics and mechanism of the antiepileptic drug oxcarbazepine (OXC) by UV-activated persulfate oxidation were investigated in this study. Results showed that UV/persulfate (UV/PS) process appeared to be more effective in degrading OXC than UV or PS alone. The OXC degradation exhibited a pseudo-first order kinetics pattern and the degradation rate constants (k obs) were affected by initial OXC concentration, PS dosage, initial pH, and humic acid concentration to different degrees. It was found that low initial OXC concentration, high persulfate dosage, and initial pH enhanced the OXC degradation. Additionally, the presence of humic acid in the solution could greatly inhibit the degradation of OXC. Moreover, hydroxyl radical (OH•) and sulfate radical (SO4 (-)••) were identified to be responsible for OXC degradation and SO4 (-)• made the predominant contribution in this study. Finally, major intermediate products were identified and a preliminary degradation pathway was proposed. Results demonstrated that UV/PS system is a potential technology to control the water pollution caused by emerging contaminants such as OXC.


Asunto(s)
Carbamazepina/análogos & derivados , Sulfatos/química , Sulfatos/efectos de la radiación , Rayos Ultravioleta , Contaminantes Químicos del Agua/química , Anticonvulsivantes/química , Carbamazepina/química , Radical Hidroxilo/química , Cinética , Oxcarbazepina , Oxidación-Reducción , Fotólisis
11.
J Environ Manage ; 156: 266-75, 2015 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-25889275

RESUMEN

This work reports on the removal and mineralization of an endocrine disrupting chemical, Bisphenol A (BPA) at a concentration of 0.22 mM in aqueous solution using inorganic oxidants (hydrogen peroxide, H2O2 and sodium persulfate, Na2S2O8;S2O8(2-)) under UV irradiation at a wavelength of 254 nm and 40 W power (Io = 1.26 × 10(-6) E s(-1)) at its natural pH and a temperature of 29 ± 3 °C. With an optimum persulfate concentration of 1.26 mM, the UV/S2O8(2-) process resulted in ∼95% BPA removal after 240 min of irradiation. The optimum BPA removal was found to be ∼85% with a H2O2 concentration of 11.76 mM. At higher concentrations, either of the oxidants showed an adverse effect because of the quenching of the hydroxyl or sulfate radicals in the BPA solution. The sulfate-based oxidation process could be used over a wider initial pH range of 3-12, but the hydroxyl radical-based oxidation of BPA should be carried out in the acidic pH range only. The water matrix components (bicarbonate, chloride and humic acid) showed higher scavenging effect in hydroxyl radical-based oxidation than that in the sulfate radical-based oxidation of BPA. UV/S2O8(2-) oxidation system utilized less energy (307 kWh/m(3)) EE/O in comparison to UV/H2O2 system (509 kWh/m(3)) under optimum operating conditions. The cost of UV irradiation far outweighed the cost of the oxidants in the process. However, the total cost of treatment of persulfate-based system was much lower than that of H2O2-based oxidation system.


Asunto(s)
Compuestos de Bencidrilo/química , Disruptores Endocrinos/química , Fenoles/química , Rayos Ultravioleta , Contaminantes Químicos del Agua/química , Contaminación Química del Agua/prevención & control , Purificación del Agua/métodos , Compuestos de Bencidrilo/efectos de la radiación , Bicarbonatos , Cloruros , Sustancias Húmicas , Peróxido de Hidrógeno/efectos de la radiación , Oxidantes Fotoquímicos/efectos de la radiación , Oxidación-Reducción , Fenoles/efectos de la radiación , Compuestos de Sodio/efectos de la radiación , Sulfatos/efectos de la radiación , Contaminantes Químicos del Agua/efectos de la radiación
12.
Talanta ; 135: 27-33, 2015 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-25640122

RESUMEN

A new chemiluminescence (CL) flow method for persulfate determination was developed based on luminol oxidation by in-line generated radicals. Reactive oxygen species (ROS) generated by CdTe quantum dots (QDs) under a low energetic radiation (visible light emitted by LEDs) promoted the decomposition of persulfate ion (S2O8(2-)) into sulfate radical (SO4(∙-)), leading to subsequent radical chain reactions that yield the emission of light. Due to the inherent radical short lifetimes and the transient behavior of CL phenomena an automated multi-pumping flow system (MPFS) was proposed to improve sample manipulation and reaction zone implementation ensuring reproducible analysis time and high sampling rate. The developed approach allowed up to 60 determinations per hour and determine S2O8(2-) concentrations between 0.1 and 1 mmol with good linearity (R=0.9999). The method has shown good repeatability with relative standard deviations below 2.5% (n=3) for different persulfate concentrations (0.1 and 0.625 mmol L(-1)). Limits of detection (3σ) and quantification (10σ) were 2.7 and 9.1 µmol L(-1), respectively. The MPFS system was applied to persulfate determination in bench scale UV/S2O8(2-) drug degradation processes of model samples showing good versatility and providing real time information on the persulfate consumption in photo-chemical degradation methodologies.


Asunto(s)
Ácido 3-Mercaptopropiónico/efectos de la radiación , Compuestos de Cadmio/efectos de la radiación , Luminol/química , Compuestos de Potasio/efectos de la radiación , Puntos Cuánticos/efectos de la radiación , Especies Reactivas de Oxígeno/química , Sulfatos/efectos de la radiación , Telurio/efectos de la radiación , Ácido 3-Mercaptopropiónico/química , Compuestos de Cadmio/química , Luz , Nanopartículas/química , Oxidación-Reducción , Compuestos de Potasio/química , Puntos Cuánticos/química , Sulfatos/química , Telurio/química
13.
J Hazard Mater ; 279: 375-83, 2014 Aug 30.
Artículo en Inglés | MEDLINE | ID: mdl-25086235

RESUMEN

The extensive production and usage of antibiotics have led to an increasing occurrence of antibiotic residuals in various aquatic compartments, presenting a significant threat to both ecosystem and human health. This study investigated the degradation of selected ß-lactam antibiotics (penicillins: ampicillin, penicillin V, and piperacillin; cephalosporin: cephalothin) by UV-254nm activated H2O2 and S2O8(2-) photochemical processes. The UV irradiation alone resulted in various degrees of direct photolysis of the antibiotics; while the addition of the oxidants improved significantly the removal efficiency. The steady-state radical concentrations were estimated, revealing a non-negligible contribution of hydroxyl radicals in the UV/S2O8(2-) system. Mineralization of the ß-lactams could be achieved at high UV fluence, with a slow formation of SO4(2-) and a much lower elimination of total organic carbon (TOC). The transformation mechanisms were also investigated showing the main reaction pathways of hydroxylation (+16Da) at the aromatic ring and/or the sulfur atom, hydrolysis (+18Da) at the ß-lactam ring and decarboxylation (-44Da) for the three penicillins. Oxidation of amine group was also observed for ampicillin. This study suggests that UV/H2O2 and UV/S2O8(2-) advanced oxidation processes (AOPs) are capable of degrading ß-lactam antibiotics decreasing consequently the antibiotic activity of treated waters.


Asunto(s)
Antibacterianos/química , Peróxido de Hidrógeno/química , Compuestos de Sodio/química , Sulfatos/química , beta-Lactamas/química , Antibacterianos/análisis , Peróxido de Hidrógeno/efectos de la radiación , Radical Hidroxilo/química , Cinética , Fotólisis , Compuestos de Sodio/efectos de la radiación , Sulfatos/efectos de la radiación , Rayos Ultravioleta , beta-Lactamas/análisis
14.
ChemSusChem ; 7(1): 127-34, 2014 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-24155063

RESUMEN

Chemical and visible-light-driven water oxidation catalyzed by a number of Ni complexes and salts have been investigated at pH 7-9 in borate buffer. For chemical oxidation, [Ru(bpy)3](3+) (bpy = 2,2'-bipyridine) was used as the oxidant, with turnover numbers (TONs) >65 and a maximum turnover frequency (TOFmax) >0.9 s(-1). Notably, simple Ni salts such as Ni(NO3 )2 are more active than Ni complexes that bear multidentate N-donor ligands. The Ni complexes and salts are also active catalysts for visible-light-driven water oxidation that uses [Ru(bpy)3](2+) as the photosensitizer and S2 O8 (2-) as the sacrificial oxidant; a TON>1200 was obtained at pH 8.5 by using Ni(NO3)2 as the catalyst. Dynamic light scattering measurements revealed the formation of nanoparticles in chemical and visible-light-driven water oxidation by the Ni catalysts. These nanoparticles aggregated during water oxidation to form submicron particles that were isolated and shown to be partially reduced ß-NiOOH by various techniques, which include SEM, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, XRD, and IR spectroscopy. These results suggest that the Ni complexes and salts act as precatalysts that decompose under oxidative conditions to form an active nickel oxide catalyst. The nature of this active oxide catalyst is discussed.


Asunto(s)
Complejos de Coordinación/química , Níquel/química , Agua/química , Catálisis , Complejos de Coordinación/efectos de la radiación , Luz , Nanopartículas del Metal/química , Níquel/efectos de la radiación , Compuestos Organometálicos/química , Compuestos Organometálicos/efectos de la radiación , Oxidación-Reducción , Rutenio/química , Rutenio/efectos de la radiación , Sales (Química)/química , Compuestos de Sodio/química , Compuestos de Sodio/efectos de la radiación , Sulfatos/química , Sulfatos/efectos de la radiación
15.
Artículo en Inglés | MEDLINE | ID: mdl-23802163

RESUMEN

The aim of this research was development of new system for the treatment of highly polluted wastewater (COD = 10240 mg/L; SS = 2860 mg/L) originating from vine-making industry. The system consisted of the main treatment that included electrochemical methods (electro oxidation, electrocoagulation using stainless steel, iron and aluminum electrode sets) with simultaneous sonication and recirculation in strong electromagnetic field. Ozonation combined with UV irradiation in the presence of added hydrogen peroxide was applied for the post-treatment of the effluent. Following the combined treatment, the final removal efficiencies of the parameters color, turbidity, suspended solids and phosphates were over 99%, Fe, Cu and ammonia approximately 98%, while the removal of COD and sulfates was 77% and 62%, respectively. A new approach combining electrochemical methods with ultrasound in the strong electromagnetic field resulted in significantly better removal efficiencies for majority of the measured parameters compared to the biological methods, advanced oxidation processes or electrocoagulation. Reduction of the treatment time represents another advantage of this new approach.


Asunto(s)
Peróxido de Hidrógeno/química , Ozono/química , Rayos Ultravioleta , Eliminación de Residuos Líquidos/métodos , Contaminantes del Agua/química , Contaminantes del Agua/efectos de la radiación , Amoníaco/química , Amoníaco/efectos de la radiación , Análisis de la Demanda Biológica de Oxígeno , Cobre/química , Cobre/efectos de la radiación , Electroquímica/métodos , Hierro/química , Hierro/efectos de la radiación , Nefelometría y Turbidimetría , Oxidantes/química , Oxidación-Reducción , Fosfatos/química , Fosfatos/efectos de la radiación , Sonicación , Sulfatos/química , Sulfatos/efectos de la radiación , Aguas Residuales , Vino
16.
Radiat Prot Dosimetry ; 152(4): 400-5, 2012 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-22628526

RESUMEN

In this study, an approximate symmetric cylindrical manganese bath system with equal diameter and height was appraised using a Monte Carlo simulation. For nine sizes of the tank filled with MnSO(4).H(2)O solution of three different concentrations, the necessary correction factors involved in the absolute measurement of neutron emission rate were determined by a detailed modelling of the MCNP4C code with the ENDF/B-VII.0 neutron cross section data library. The results obtained were also used to determine the optimum dimensions of the bath for each concentration of solution in the calibration of (241)Am-Be and (252)Cf sources. Also, the amount of gamma radiation produced as a result of (n,γ) the reaction with the nuclei of the manganese sulphate solution that escaped from the boundary of each tank was evaluated. This gamma can be important for the background in NaI(Tl) detectors and issues concerned with radiation protection.


Asunto(s)
Algoritmos , Compuestos de Manganeso/química , Compuestos de Manganeso/efectos de la radiación , Modelos Estadísticos , Método de Montecarlo , Radiometría/métodos , Sulfatos/química , Sulfatos/efectos de la radiación , Simulación por Computador , Neutrones , Dosis de Radiación , Dispersión de Radiación
17.
Ultrason Sonochem ; 19(3): 469-74, 2012 May.
Artículo en Inglés | MEDLINE | ID: mdl-22079807

RESUMEN

Degradation of the antibiotics amoxicillin in aqueous solution using sulphate radicals under ultrasound irradiation was investigated. The preliminary studies of optimal degradation methodology were conducted with only oxone (2KHSO(5) · KHSO(4) · K(2)SO(4)), cobalt activated oxone (oxone/Co(2+)), oxone+ultrasonication (oxone/US) and cobalt activated oxone+ultrasonication (oxone/Co(2+)/US). The chemical oxygen demand (COD) removal efficiency were in the order of oxone

Asunto(s)
Amoxicilina/química , Sonicación/métodos , Sulfatos/química , Sulfatos/efectos de la radiación , Contaminantes Químicos del Agua/química , Purificación del Agua/métodos , Agua/química , Amoxicilina/aislamiento & purificación , Amoxicilina/efectos de la radiación , Radicales Libres/química , Radicales Libres/efectos de la radiación , Ondas de Choque de Alta Energía , Dosis de Radiación , Soluciones , Contaminantes Químicos del Agua/aislamiento & purificación , Contaminantes Químicos del Agua/efectos de la radiación
18.
Ultrason Sonochem ; 17(5): 752-5, 2010 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-20226709

RESUMEN

Mild and efficient Fischer esterification reactions of lactic acid with a variety of straight chain aliphatic alcohols, cyclohexanol and benzyl alcohol were successfully performed using two novel Brønsted acidic ionic liquids that bear an aromatic sulfonic acid group on the imidazolium or pyridinium cation under ultrasound irradiation. These reactions carried out smoothly with good to excellent conversion rate (78-96%) and satisfactory yields (73-92%) in shorter reaction time (4-6h) at room temperature when the amount of ionic liquids was 20 mol%. These ionic liquids could be recovered readily and recycled five times without any significant loss in their catalytic activity.


Asunto(s)
Líquidos Iónicos/química , Líquidos Iónicos/efectos de la radiación , Ácido Láctico/síntesis química , Ácido Láctico/efectos de la radiación , Sonicación , Sulfatos/química , Sulfatos/efectos de la radiación , Ácidos/química , Ácidos/efectos de la radiación , Ésteres/química , Ésteres/efectos de la radiación , Solventes/química , Solventes/efectos de la radiación
19.
Biomed Mater ; 3(3): 034121, 2008 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-18765896

RESUMEN

Nano-sized calcium deficient hydroxyapatite (CDHA) powders with an average particle size less than 100 nm were prepared by a co-precipitation method at low temperature. The initial Ca/P molar ratio was chosen to be less than the stoichiometric ratio of beta-TCP (1.5). Additionally, lowering the temperature and pH values accelerated HPO(4)(2-) incorporation in the CDHA structure. HPO(4)(2-) is considered as an essential source for beta-TCP formation. Sulfate ion doping during the maturation period is proved to be an effective step to eliminate the pyrophosphate P(2)O(7)(2-) phase that results during the calcination of CDHA with Ca/P < 1.5. Furthermore, the heating effect of microwave irradiation resulted in an increase in Ca ion concentration and lowered the CDHA deficiency which affected beta-TCP purity despite its ability to reduce the particle size. A purity of 99.32% beta-TCP with respect to the P(2)O(7)(2-) phase was achieved by increasing the sulfate ion concentration from 2% to 3% and the calcination temperatures from 900 degrees C to 1100 degrees C.


Asunto(s)
Sustitutos de Huesos/química , Fosfatos de Calcio/química , Nanoestructuras/química , Nanoestructuras/ultraestructura , Sulfatos/química , Implantes Absorbibles , Absorción , Líquidos Corporales/química , Sustitutos de Huesos/efectos de la radiación , Fosfatos de Calcio/efectos de la radiación , Elasticidad/efectos de la radiación , Dureza/efectos de la radiación , Iones , Ensayo de Materiales , Microondas , Nanoestructuras/efectos de la radiación , Tamaño de la Partícula , Dosis de Radiación , Sulfatos/efectos de la radiación
20.
Anal Chem ; 79(12): 4455-62, 2007 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-17500533

RESUMEN

This paper investigates the thermal and irradiation-dependent dehydration and kinetics occurring in Na2SO4.10H2O (mirabilite) and MgSO4.7H2O (epsomite) at room conditions by using powder X-ray thermodiffraction. An improved version of a first optically stimulated X-ray diffractometer prototype was used. Specific software for the thermodiffraction study was developed (XPowder PLUS) and a filter inserted between the lamp (heating system) and the sample. The results show that these salts are thermal and irradiation sensitive. The temperature and kinetic rates of the salt conversions differed depending on direct exposure to high-intensity radiation (photodehydration) or whether the radiation was blocked by the filter (thermodehydration). In general, radiation-induced dehydration triggers the transformation at lower temperature and accelerates the kinetic reaction more than when the filter is used. Mirabilite dehydration starts with the initial radiation impacts, unlike epsomite. Thermodehydration and photodehydration of mirabilite is a non-isothermal reaction occurring through an amorphous-mediated step. Radiation damage in epsomite leads to isothermal dehydration, whereas non-isothermal dehydration occurs when epsomite is thermally damaged. In both cases, no amorphous material was observed. Because of the weaker bond between cation and oxygen atom in mirabilite, its thermal and radiation stability is lower than in epsomite. These results have important implications for the prevention of salt weathering of porous materials found in the cultural heritage.


Asunto(s)
Deshidratación , Rayos Infrarrojos , Sulfato de Magnesio/química , Sulfatos/química , Difracción de Rayos X , Cinética , Sulfato de Magnesio/efectos de la radiación , Sulfatos/efectos de la radiación , Temperatura
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