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1.
Mar Pollut Bull ; 197: 115793, 2023 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-37984094

RESUMEN

Sanmen Bay plays a crucial role in economic shellfish aquaculture in China, yet few studies exist on the arsenic speciation of shellfish from this area. In this study, arsenic speciation of 11 cultured shellfish species from Sanmen Bay were analyzed by HPLC/ICP-MS. The results showed that organic arsenic particularly AsB, was the dominant arsenic species, constituting 21 %-71 % of the total arsenic. Conversely, the levels of inorganic arsenic were relatively low, ranging from 0.007 to 0.093 mg/kg, only accounted for 0.2 %-5.7 % of the total arsenic. There was no significant level correlation between inorganic arsenic and total arsenic in Sanmen Bay shellfish, so the concentration of inorganic arsenic did not increase with the total arsenic. Overall, the present study firstly revealed the arsenic speciation of shellfish from Sanmen Bay and also suggested that the proportion of inorganic arsenic should be considered in the revision of arsenic limit values.


Asunto(s)
Arsénico , Arsenicales , Arsénico/análisis , Arsenicales/análisis , Bahías , China , Mariscos/análisis , Animales
2.
BMC Vet Res ; 18(1): 122, 2022 Mar 31.
Artículo en Inglés | MEDLINE | ID: mdl-35361203

RESUMEN

BACKGROUND: Eugenol is the most commonly used plant anesthetic to relieve the stressors during various aquaculture procedures. This study aims to investigate the pharmacokinetics of eugenol in Pacific white shrimp by immersion baths in a simulated transportation. RESULTS: The pharmacokinetics of eugenol were firstly investigated in Pacific white shrimp by immersion baths of 300 mg L- 1 eugenol over 5 min (Treatment 1), 10 mg L- 1 eugenol during 24 h (Treatment 2) and a sequential immersion administration (Treatment 3). Concentrations of eugenol in hemolymph, hepatopancreas, and muscle were determined using Gas chromatography-tandem mass spectrometry (GC-MS/MS). After immersion bath of Treatment 1, the elimination half-life (t1/2z) values are 1.3 h and 11 h for hepatopancreas and muscles, indicating the rapid absorption and elimination of eugenol in shrimp. Under the Treatment 2 administration, the eugenol peak concentration is 6527.9 µg/kg in muscle, followed by 402.8 µg/kg in hepatopancreas, with the lowest concentration of 37.9 µg/L in hemolymph. Area under the curve (AUC0-∞) values lie in the order of muscle > hepatopancreas > hemolymph, suggesting that eugenol tends to accumulate in muscle by the immersion administration. Moreover, the average residence time (MRT0-∞) values of 38.6, 23.0 and 115.3 h for hemolymph, hepatopancreas and muscle are achieved, which may indicate that hepatopancreas is the main organ for elimination of eugenol. After combining the conditions in a sequential bath immersion of eugenol (Treatment 3), the maximum concentration (Cmax) values of eugenol are higher than those achieved in Treatment 2, indicating that accumulation of eugenol happened in haemolymph, hepatopancreas and muscle. In addition, the corresponding t1/2z values are 4.7, 14.9 and 47.6 h, respectively, suggesting the faster elimination from the tissues following sequential administration. After the immersion bath, eugenol concentrations in muscle of Pacific white shrimp are lower than 2.5 mg/kg at 2 h, 48 h and 24.5 h in Treatment 1 ~ 3. CONCLUSIONS: A withdrawal period of 2 h, 48 h and 24.5 h following a 300 mg L- 1 of eugenol over a 5-min, 10 mg L- 1 eugenol concentration during a 24-h and combined conditions in a sequential immersion bath were suggested.


Asunto(s)
Eugenol , Penaeidae , Animales , Eugenol/farmacocinética , Cromatografía de Gases y Espectrometría de Masas/veterinaria , Inmersión , Espectrometría de Masas en Tándem/veterinaria
3.
Sci Total Environ ; 802: 149891, 2022 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-34474296

RESUMEN

Animals exposure to polychlorinated biphenyls (PCBs) may result in retention of hydroxylated PCBs (OH-PCBs). OH-PCBs can be accumulated in animals, including humans, through the transmission of food chain. However, there are few studies on the accumulation and metabolism of OH-PCBs exposed to the body through daily diet. Therefore, this study was conducted to investigate the fate of OH-PCBs after being ingested through dietary intake. By adding 3-OH-PCB101 and 4-OH-PCB101 to the edible tissue of crucian carp, which were used as raw materials to prepare mouse feed, with an exposure concentration of 2.5 µg/kg ww. The exposure experiment lasted for a total of 80 days. The blood, feces and 11 tissues of mice at different times were analyzed qualitatively and quantitatively. It was found that major OH-PCB101 were accumulated in intestine or excreted with feces. A small part was accumulated in heart, lung and spleen. For the first time that the conversion from OH-PCB101 to PCB101 in mice was discovered, which shows from another perspective that persistent organic pollutants are difficult to be completely degraded in the environment. 4-MeO-PCB101, 3-MeSO2-PCB101, and 4-MeSO2-PCB101 were also found in various tissues. The results of this study show that after OH-PCBs accumulated in animals re-enter the organism through the food chain, they can be metabolized again and may be reversely transformed into the parent compounds. The present research shed new light on simulating the metabolic transformation process of OH-PCBs exposed to mammals through ingestion of fish. Available data show that second-generation persistent organic pollutants in the environment still need to be continuously concerned.


Asunto(s)
Contaminantes Ambientales , Bifenilos Policlorados , Animales , Dieta , Peces , Hidroxilación , Ratones , Bifenilos Policlorados/análisis
4.
Environ Res ; 204(Pt A): 111958, 2022 03.
Artículo en Inglés | MEDLINE | ID: mdl-34478721

RESUMEN

There exist two common processes in fishery culture, i.e. antibiotic addition to reduce disease in fishery, and chlorination disinfection to inhibit infectious pathogenic microorganisms. However, antibiotic residues might play important reverse side roles for both aquaculture water pollution and potential formation of chlorination side products. Herein, the transformation behaviour, intermediates analyses and conversion pathway of antibiotic sulfamethoxazole (SMX), and potential generation of halogenated acetic acids (HAAs) in the process of chlorination in fishery water were examined, and the results revealed that the decomposing of SMX satisfied a pseudo first-order kinetic equation. Both the addition of available chlorine and high temperature had affirmative influences on the decontamination of SMX and production of HAAs, and the near-neutral pHs promoted the removal of SMX and generation of HAAs. Br- was favorable for the removal of SMX and yields of brominated acetic acids (Br-AAs). Based on the identified intermediate products, the transformation path of SMX in chlorination process was propounded, to wit, the C-S and S-N bonds in the SMX molecules were firstly cracked, and the primeval intermediate groups are then transformed to form chloroanilines, chlorophenols, etc., and subsequently, chlorophenols were chlorinated and ring-opened to generate toxic HAAs. This study might be meaningful to evaluate the effective removal of sulfonamide antibiotic residues and the potential generation of halogenated DBPs (H-DBPs) when chlorinated in aquaculture water.


Asunto(s)
Desinfectantes , Contaminantes Químicos del Agua , Purificación del Agua , Acuicultura , Cloro , Desinfectantes/análisis , Desinfección , Halogenación , Sulfametoxazol , Trihalometanos , Agua , Contaminantes Químicos del Agua/análisis
5.
Se Pu ; 39(12): 1340-1346, 2021 Dec.
Artículo en Chino | MEDLINE | ID: mdl-34812006

RESUMEN

Determination of fatty acid compositions and contents in Chinese mitten crabs is of great significance to evaluate its nutritional value and quality. However, in the face of a wide range of fatty acid extraction and methyl esterification reagents, the measurement results are uneven, and it is difficult to accurately quantify the rich fatty acids in Chinese mitten crabs. In this paper, four kinds of oil extraction reagents and two kinds of methylating reagents, were investigated. Chloroform-methanol (1∶1, v/v) was used as the extraction solvent, and methanol containing 2% sulfuric acid was used as the derivatization reagent. A method for the determination of fatty acids in the muscle of Chinese mitten crabs by gas chromatography was established. The experiment was carried out under the condition of programmed temperature rise, 37 kinds of fatty acids were separated on a DM-2560 capillary column (100 m×0.25 mm×0.20 µm), detected by hydrogen flame ionization detector (FID) and quantified by external standard method. The linear relationships of the 37 fatty acids were good in the range of 0.5-100.0 µg/mL. The correlation coefficients (R2) were 0.9981-0.9999. The limits of detection (LODs) and limits of quantification (LOQs) were 0.01-0.02 mg/100 g and 0.04-0.06 mg/100 g, respectively. The methodology was validated by palmitic acid and stearic acid. The recoveries were 76.0%-97.5%, and the relative standard deviations (RSD, n=5) were 3.31%-7.90% at the spiked levels of 1, 2 and 10 mg/100 g. The method was applied to the determination of fatty acid compositions and contents in the muscle of Chinese mitten crabs. A total of 31 kinds of fatty acids were detected. The length of carbon chain ranged from 12 to 24, and the total content of fatty acids reached 281.03 mg/100 g. Oleic acid, docosahexaenoic acid and eicosapentaenoic acid were the main fatty acids in the muscle of Chinese mitten crabs. Thus, this method provided accurate and reliable theoretical data for the determination of fatty acids in Chinese mitten crabs. This method has the advantages of simple operation, small amount of reagent and sample, reliable qualitative, accurate quantitative, detection of more fatty acid types. It is suitable for the rapid detection of fatty acid compositions and contents in muscle tissue of Chinese mitten crabs.


Asunto(s)
Ácidos Grasos , China , Cromatografía de Gases , Ionización de Llama , Cromatografía de Gases y Espectrometría de Masas
6.
Molecules ; 26(16)2021 Aug 17.
Artículo en Inglés | MEDLINE | ID: mdl-34443562

RESUMEN

A sensitive and reliable method was developed to determine methylene blue (MB) and its metabolite residues, including azure A (AZA), azure B (AZB), and azure C (AZC) in aquatic products by HPLC-MS/MS. The samples were extracted by acetonitrile and cleaned up by alumina-neutral (ALN) cartridges. The analytes were separated on a Sunfire C18 column (150 mm × 2.1 mm, 5 µm). The method was validated according to the European criteria of Commission Decision 2002/657/CE. Good linearity between 1-500 µg/L was obtained with correlation coefficients (R2) greater than 0.99. The limit of quantification (LOQ) was 1.0 µg/kg. The average recoveries at three levels of each compound (1, 5, and 10 µg/kg) were demonstrated to be in the range of 71.8-97.5%, with relative standard deviations (RSDs) from 1.05% to 8.63%. This method was suitable for the detection of methylene blue and its metabolite residues in aquatic products.


Asunto(s)
Cromatografía Líquida de Alta Presión , Azul de Metileno/análisis , Espectrometría de Masas en Tándem , Residuos de Medicamentos/análisis , Residuos de Medicamentos/metabolismo , Límite de Detección , Modelos Lineales , Azul de Metileno/metabolismo
7.
Food Chem ; 361: 130044, 2021 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-34049048

RESUMEN

A method for the determination of 8 biogenic amines in aquatic products and their derived products was established by HPLC-MS/MS without derivatization. The samples were extracted by 5% perchloric acid solution. N-hexane was used to clean the extract. The analytes were separated by a column of ACQUITY UPLC HSS T3 (100 mm × 2.1 mm, 1.8 µm), and gradient eluted with a mixed solution of (0.5% formic acid) and acetonitrile. Good linearity was obtained with correlation coefficients (R2) >0.99. This method achieved higher sensitivity (from 0.1 mg/kg for tyramine, 2-phenylethylamine and tryptamine to 1.0 mg/kg for spermidine, spermine, cadaverin, histamine and putrescine). The average recoveries were demonstrated in the range of 70.9%-113.1%, with relative standard deviations (RSDs) from 0.33% to 10.81%. This method was suitable for the detection of BAs in aquatic products and their products.


Asunto(s)
Aminas Biogénicas/análisis , Cromatografía Líquida de Alta Presión/métodos , Alimentos Marinos/análisis , Espectrometría de Masas en Tándem/métodos , Cadaverina/análisis , Histamina/análisis , Fenetilaminas/análisis , Putrescina/análisis , Espermidina/análisis , Espermina/análisis , Triptaminas/análisis , Tiramina/análisis
8.
RSC Adv ; 11(24): 14746-14754, 2021 Apr 15.
Artículo en Inglés | MEDLINE | ID: mdl-35423964

RESUMEN

Antibiotic addition and chlorination are two common processes in fishery culture. Antibiotic residues not only pollute aquaculture water, but are also one of the potential precursors of disinfection by-products (DBPs) during chlorination. The degradation kinetics, products identification and reaction mechanism of sulfacetamide (SFA), a new sulfonamides antibiotics, and potential formation of haloacetic acids (HAAs) in chlorination were explored. The results showed that the degradation of SFA followed pseudo first-order kinetic model, and chlorinating agent dose, pH of water, water temperature, NH4 +, HCO3 - and humic acid (HA) had various effects on the degradation of SFA and the yields of HAAs. The presence of Br- accelerated both the degradation rate of SFA and more formation of Br-DBPs. Through the identification of intermediate products, we proposed the transformation pathway of SFA during the chlorination disinfection process. Namely, in this NaClO disinfection system, the C-S bond between the sulfonyl group and benzene ring, and S-N bond between sulfonyl and acylamino of SFA were broken, and then the primary formed groups were further oxidized to produce intermediates, such as chloroanilines and chlorophenols. And then chlorophenols were subsequently chlorinated to form toxic HAAs. The present study might be of significance for the evaluation of effective degradation of SFA and potential production of halogenate-DBPs (H-DBPs) during the chlorination disinfection process in aquaculture water.

9.
J Hazard Mater ; 399: 123090, 2020 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-32526426

RESUMEN

Strategies to maximize the reuse of electronic and industrial wastes have scientific, economic, social and environmental implications. We herein propose a strategy of "treating waste with waste" using LiCoO2 cathode powders from spent lithium ion batteries to eliminate industrial pollutants led by sulfur (S) (IV) in waste water. By radical scavenging experiments and electron spin resonance (ESR) analysis, we identified singlet 1O2 as the dominant species while SO4- and OH as the secondary species for decontamination during the oxidization process mediated by LiCoO2 powders. The intrinsic mechanism of S(IV) conversion was revealed to be two-step hydrogen migrations from HSO3- to O2 occurring on LiCoO2 surface by density functional theory (DFT) calculations. The surface of LiCoO2 powders plays a key role in anchoring sulfur species and forming surface complex as an excellent medium, which is found to be stable and reusable by material characterizations and the recycling experiment. Free Co(II) ions in solvents have no catalysis effect on the conversion of pollutants. Our work offers a particularly vivid example for rational reuse of electronic wastes to eliminate industrial pollutants, and may raise economic benefits in environmental practice due to two aims achieved in once action.

10.
Chirality ; 32(3): 324-333, 2020 03.
Artículo en Inglés | MEDLINE | ID: mdl-31877236

RESUMEN

A simple and sensitive method has been established based on pass-through cleanup and high-performance liquid chromatography quadrupole-orbitrap mass spectrometry (HPLC-Q/Orbitrap MS) for the simultaneous determination of ten aminoglycosides (AGs) in aquatic feeds. The extraction solution and cleanup procedure had been optimized, and good sensitivity, accuracy, and precision were obtained. The calibration curves of AGs were linearity (R2 > 0.99) in the range of 2.0 to 200 µg/L (or 5.0 to 500 µg/L). The limits of detection of AGs were between 10 and 25 µg/kg. The recoveries of AGs ranged from 74.9% to 94.3%, and the intraday and interday relative standard deviations were less than 15%. Finally, this method was successfully applied to determine ten AGs in 30 aquatic feed samples. It might be the first time to use pass-through cleanup approach combined with HPLC-Q/Orbitrap MS method for AGs determination in aquatic feed samples.


Asunto(s)
Aminoglicósidos/análisis , Alimentación Animal/análisis , Antibacterianos/análisis , Cromatografía Líquida de Alta Presión/métodos , Espectrometría de Masas/métodos , Aminoglicósidos/química , Animales , Antibacterianos/química , Calibración , China , Crustáceos/química , Peces , Límite de Detección , Reproducibilidad de los Resultados
11.
Chemosphere ; 199: 84-88, 2018 May.
Artículo en Inglés | MEDLINE | ID: mdl-29433031

RESUMEN

Both Cl- and base can affect PMS activation to produce reactive chlorine or oxygen species, but the overall effects of chloride on this emerging PMS/base technology in saline wastewater treatment are unknown. Here effectiveness of PMS/base, PMS/Cl- and PMS/base/Cl- is compared with a gradient concentration of chloride and alkalinity, by probing the degradation of methylene blue (MB). Both PMS/base and PMS/Cl- systems can rapidly degrade MB due to the generation of singlet oxygen and reactive chlorine, respectively. Interestingly, dye degradation and adsorbable organic halides (AOX) formation are inhibited in the PMS/base/Cl- system as high concentrations of Cl- and base co-exist. Reaction of PMS with chloride diminishes the effective concentration of PMS by base activation, whereas in return high alkalinity decreases the oxidation capacity of reactive species. Therefore, this finding may have significant technical implications for evaluating the applicability of the emerging PMS/base technology and optimizing the conditions for AOX abatement in PMS-based processes.


Asunto(s)
Peróxidos/farmacología , Aguas Residuales/química , Purificación del Agua/métodos , Adsorción , Cloruros/química , Cloro , Oxidación-Reducción
12.
Chemosphere ; 182: 624-629, 2017 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-28527415

RESUMEN

Trace bromide (Br-) released from industrial effluents or brominated compounds is able to directly react with peroxymonosulfate (PMS) to generate a series of reactive oxidants which can oxidize and also halogenate organics. We report the identification and evolution of by-products during 2,4,6-trichlorophenol (TCP) degradation in the presence of PMS and trace Br-. The influencing factors, including Br- concentration and pH, were investigated. The depletion of TCP was accelerated with increasing trace Br- concentration (0-0.2 mM) and was affected by the initial pH (3.0-7.0). The chlorinated and brominated compounds were identified in simulated wastewater during treatment with PMS. Notably, the potential formation of chlorobromoaromatic by-products was demonstrated for the first time in the presence of PMS and trace Br-. The possible reaction pathways of TCP and its derivatives are discussed. These findings have important implications for the future applications of PMS-based oxidation processes.


Asunto(s)
Bromuros/química , Clorofenoles/química , Restauración y Remediación Ambiental/métodos , Peróxidos/química , Contaminantes Químicos del Agua/química , Halogenación , Concentración de Iones de Hidrógeno , Oxidación-Reducción , Investigación , Aguas Residuales/química
13.
Chemosphere ; 173: 529-534, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-28142111

RESUMEN

Base activation of peroxydisulfate (PDS) is a common process aiming for water treatment, but requires high doses of PDS and strongly basic solutions. Peroxymonosulfate (PMS), another peroxygen of sulfurate derived from PDS, may also be activated by a less basic solution. However, enhancing the base-PMS reactivity is still challenging. Here it is reported that pyrophosphate (PA) and tripolyphosphate (PB) can efficiently enhance PMS activation under weakly alkaline conditions (pH 9.5) via the formation of superoxide anion radical (O2•-) and singlet oxygen (1O2). The rate constant of Acid Orange 7 (AO7) degradation in PA/PMS system (kPA/PMS) was nearly 4.4-15.9 fold higher than that in PMS/base system (kPMS/base) without any polyphosphates. Increases in PA (or PB) concentration, PMS dose and pH favored the rapid dye degradation. Gas chromatograph-mass spectrometer (GC-MS) data confirmed AO7 and 2,4,6-trichlorophenol (2,4,6-TCP) were decomposed to a series of organic intermediates. The radical quenching and probe oxidation experiments indicate the degradation of organic compounds in the PA/PMS and PB/PMS processes was not reliant on sulfate radical (SO4•-) and hydroxyl radical (OH) species but on O2- and 1O2 reactive species. Comparison experiments show that the polyphosphate/PMS process was much more favorable than PDS/base process. The present work provides a novel way to activate PMS for contaminant removal using industrial polyphosphate wastewaters.


Asunto(s)
Radical Hidroxilo/química , Peróxidos/química , Polifosfatos/farmacología , Sulfatos/química , Aguas Residuales/química , Contaminantes Químicos del Agua/aislamiento & purificación , Purificación del Agua/métodos , Cinética , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis
14.
Environ Sci Pollut Res Int ; 23(5): 4778-85, 2016 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-26538259

RESUMEN

This study compared the behaviors of two classic advanced oxidation processes (AOPs), hydroxyl radical-based AOPs ((•)OH-based AOPs) and sulfate radical-based AOPs (SO4 (•-)-based AOPs), represented by UV/ hydrogen peroxide (H2O2) and UV/peroxydisulfate (PDS) systems, respectively, to degrade humic acid (HA) in the presence of halide ions (Cl(-) and Br(-)). The effects of different operational parameters, such as oxidant dosages, halide ions concentration, and pH on HA degradation were investigated in UV/H2O2/Cl(-), UV/PDS/Cl(-), UV/H2O2/Br(-), and UV/PDS/Br(-) processes. It was found that the oxidation capacity of H2O2 and PDS to HA degradation in the presence of halides was nearly in the same order. High dosage of peroxides would lead to an increase in HA removal while excess dosage would slightly inhibit the efficiency. Both Cl(-) and Br(-) would have depressing impact on the two AOPs, but the inhibiting effect of Br(-) was more obvious than that of Cl(-), even the concentration of Cl(-) was far above that of Br(-). The increasing pH would have an adverse effect on HA decomposition in UV/H2O2 system, whereas there was no significant impact of pH in UV/PDS process. Furthermore, infrared spectrometer was used to provide the information of degraded HA in UV/H2O2/Cl(-), UV/PDS/Cl(-), UV/H2O2/Br(-), and UV/PDS/Br(-) processes, and halogenated byproducts were identified in using GC-MS analysis in the four processes. The present research might have significant technical implications on water treatment using advanced oxidation technologies.


Asunto(s)
Sustancias Húmicas , Peróxido de Hidrógeno/química , Radical Hidroxilo/química , Sulfatos/química , Rayos Ultravioleta , Purificación del Agua , Bromuros/química , Cloruros/química , Sustancias Húmicas/efectos de la radiación , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis
15.
Chemosphere ; 144: 2415-20, 2016 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-26613359

RESUMEN

Chloride ion is known to affect on degradation kinetics in different ways during HO· and SO4(·-)-based advanced oxidation processes (AOPs). However, its effect on absorbable organic halogen (AOX) evolution and acute toxicity of treated water remains unknown, despite the importance of the two parameters in evaluating the applicability of AOPs. In the present study, Co/peroxymonosulfate (Co/PMS) and UV/hydrogen peroxide (UV/H2O2) treatment of 2,4,6-trichlorophenol was compared in terms of AOX formation, chlorinated byproducts and acute toxicity. Both Co/PMS and UV/H2O2 systems were more reactive under acidic conditions, resulting in elevated AOX levels when compared with those at neutral pH. The presence of high levels of chloride led to an accumulation and increase of AOX in the Co/PMS system. The toxicity of chlorinated byproducts was evaluated using Photobacterium phosphoreum, and the results revealed a sharp increase in acute toxicity of Co/PMS reaction solutions on addition of chloride ion. However, addition of Cl(-) had no apparent impact on AOX and toxicity of UV/H2O2 reaction solutions. These findings may have significant technical implications for selecting feasible technologies to treat high salinity wastewater.


Asunto(s)
Cloruros/química , Clorofenoles/toxicidad , Photobacterium/efectos de los fármacos , Contaminantes Químicos del Agua/toxicidad , Clorofenoles/química , Cobalto/química , Peróxido de Hidrógeno/química , Oxidación-Reducción , Peróxidos/química , Rayos Ultravioleta , Eliminación de Residuos Líquidos , Aguas Residuales/química , Contaminantes Químicos del Agua/química
16.
Chemosphere ; 134: 446-51, 2015 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-26001937

RESUMEN

Dechlorination and denitration are known to occur during the oxidative degradation of chloronitroaromatic compounds, but the possibility of re-chlorination and re-nitration of chloro and nitro groups is not assessed despite of its importance in evaluating the applicability of advanced oxidation processes (AOPs). In this study, transformation of chloro and nitro groups in degradation of 4-chloro-2-nitrophenol (4C2NP) by sulfate radical generated via Co-mediated peroxymonosulfate activation was investigated. Both chloride and nitrate ions were found as the main inorganic products of chloro and nitro groups in 4C2NP, but their levels were much lower than that of degraded parent 4C2NP. A typical dual effect of chloride on the 4C2NP degradation kinetics was observed, whereas no measurable influence was found for addition of low level nitrate. Re-chlorination took place, but re-nitration was not verified because several polychlorophenols but none of polynitrophenols were detected. The specific degradation mechanism involved in the transformation of nitro group and chloro group was proposed.


Asunto(s)
Restauración y Remediación Ambiental , Nitrofenoles/química , Oxígeno/química , Peróxidos/química , Sulfatos/química , Cloruros/análisis , Cromatografía Líquida de Alta Presión , Electrones , Monitoreo del Ambiente/métodos , Cromatografía de Gases y Espectrometría de Masas , Radical Hidroxilo/química , Residuos Industriales/análisis , Iones , Cinética , Nitrógeno/análisis , Oxidación-Reducción , Contaminantes Químicos del Agua/análisis
17.
Chemosphere ; 117: 582-5, 2014 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-25303463

RESUMEN

Activation of peroxygens is a critical method to generate oxidative species, but often consumes additional chemical reagents and/or energy. Here we report a novel and efficient activation reaction for peroxymonosulfate (PMS) by phosphate anions (PBS). The PBS/PMS coupled system, at neutral pH, is able to decompose efficiently even mineralize a variety of organic pollutants, such as Acid Orange 7, Rhodamine B and 2,4,6-trichlorophenol. In contrast, no measurable degradation was observed when the PMS was replaced by other peroxygens (i.e. hydrogen peroxide and peroxydisulfate). Both PMS and PBS are indispensable for the oxidative degradation of pollutants. Increasing pH and concentrations of PMS and PBS significantly accelerate the degradation of organics. It is proposed that OH would be the major radical for contamination degradation at pH 7.0 through the radical quenching experiments. This work provides a new way of PMS activation for decontamination at neutral pH, in particular for phosphate-rich wastewater treatment.


Asunto(s)
Compuestos Orgánicos/química , Peróxidos/química , Fosfatos/química , Contaminantes Químicos del Agua/química , Aniones/química , Clorofenoles/química , Colorantes/química , Peróxido de Hidrógeno/química , Concentración de Iones de Hidrógeno , Sulfatos/química
18.
Chemosphere ; 103: 354-8, 2014 May.
Artículo en Inglés | MEDLINE | ID: mdl-24359921

RESUMEN

The dicarboxylic acids oxalate (Oxal) and malonate (Mal) are frequently detected as the final low-molecular-weight organic acids during oxidative degradation of aromatic compounds. Here a distinct effect of Oxal versus Mal on iron-based photocatalytic technologies was reported by testing the degradation efficiency of the dye rhodamine B. The rates of dye degradation in irradiated Fe(III) solutions depended on Fe(III/II) speciation, photoreactivities of Fe complexes and reactivities of Fe(II) complexes with H2O2. Photolysis of the Fe(III)-oxalato complex was favorable due to the formation of O2-, HO2 and OH for oxidizing the dye; however, an excess of H2O2 could quench the excited state of ferrioxalate, decreasing the degradation efficiency. In contrast, activities of UV/Fe(III) in the presence of Mal were significantly diminished because Fe(III)-Mal complexes, with much lower quantum yield of Fe(II) from photoreduction, dominated Fe(III) speciation. The results provide data for an understanding of the mechanism of iron redox (photo)chemistry mediated by diacids, which will aid in selecting appropriate Fe ligands, screening photo-Fenton conditions and designing UV/Fe(III) treatability.


Asunto(s)
Compuestos Férricos/química , Compuestos Ferrosos/química , Malonatos/química , Oxalatos/química , Ácido Oxálico/química , Fotólisis , Colorantes Fluorescentes/química , Peróxido de Hidrógeno/química , Oxidación-Reducción , Rodaminas/química
19.
Environ Sci Technol ; 47(19): 11174-81, 2013 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-24015851

RESUMEN

An efficient and green advanced oxidation process (i.e., photo-sulfite reaction) for the simultaneous oxidation of sulfite and organic pollutants in water is reported. The photo-sulfite system (UV-Fe(III)-sulfite) is based on the Fe-catalyzed sulfite oxidation and photochemistry of Fe(III) species. SO4(•-) and (•)OH radicals were identified in the photo-sulfite system with radical scavenging experiments using specific alcohols. This novel technology was consistently proven to be more favorable than the alternative Fe(III)-sulfite systems for the degradation of 2,4,6-trichlorophenol (2,4,6-TCP) and other organic pollutants at all conditions tested. The reactivity of photo-sulfite system was sustained due to the spontaneous switch of photoactive species from Fe(III)-sulfito to Fe(III)-hydroxo complexes with the depletion of sulfite and the decrease in pH. In contrast, in the absence of light the performance of the Fe(III)-sulfite system was greatly diminished after the consumption of sulfite. The formation of the Fe(III)-sulfito complex is a necessary step for initiating the photo-sulfite reaction. Inhibition of the oxidation of 2,4,6-TCP and methyl orange (MO) was observed in the presence of ligands that can stabilize one or more of the reactants: Fe(III), Fe(II), or sulfite. Our study provides a new facile route for the generation of SO4(•-) and simultaneous removal of organic and inorganic pollutants.


Asunto(s)
Clorofenoles/química , Colorantes/química , Hierro/química , Sulfitos/química , Contaminantes Químicos del Agua/química , Compuestos Azo/química , Bencenosulfonatos/química , Azul de Metileno/química , Rodaminas/química , Rayos Ultravioleta
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