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1.
Environ Res ; 259: 119577, 2024 Jul 08.
Artículo en Inglés | MEDLINE | ID: mdl-38986801

RESUMEN

ß-lactam antibiotics, extensively used worldwide, pose significant risks to human health and ecological safety due to their accumulation in the environment. Recent studies have demonstrated the efficacy of transition metal-activated sulfite systems, like Fe(Ⅲ)/HSO3-, in removing PPCPs from water. However, research on their capability to degrade ß-lactam antibiotics remains sparse. This paper evaluates the degradation of 14 types of ß-lactam antibiotics in Fe(Ⅲ)/HSO3- system and establishes a QSAR model correlating molecular descriptors with degradation rates using the MLR method. Using cefazolin as a case study, this research predicts degradation pathways through NPA charge and Fukui function analysis, corroborated by UPLC-MS product analysis. The investigation further explores the influence of variables such as HSO3- dosage, substrate concentration, Fe(Ⅲ) dosage, initial pH and the presence of common seen water matrices including humic acid and bicarbonate on the degradation efficiency. Optimal conditions for cefazolin degradation in Fe(Ⅲ)/HSO3- system were determined to be 93.3 µM HSO3-, 8.12 µM Fe(Ⅲ) and an initial pH of 3.61, under which the interaction of Fe(Ⅲ) dosage with initial pH was found to significantly affect the degradation efficiency. This study not only provides a novel degradation approach for ß-lactam antibiotics but also expands the theoretical application horizon of the Fe(Ⅲ)/HSO3- system.

2.
Water Res ; 260: 121959, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38909420

RESUMEN

Combined sewer overflows (CSOs) introduce microbial contaminants into the receiving water bodies, thereby posing risks to public health. This study systematically investigated the disinfection performance and mechanisms of the combined process of ultraviolet and peracetic acid (UV/PAA) in CSOs with selecting Escherichia coli (E. coli) as a target microbial contaminant. The UV/PAA process exhibited superior performance in inactivating E. coli in simulated CSOs compared with UV, PAA, and UV/H2O2 processes. Increasing the PAA dosage greatly enhanced the disinfection efficiency, while turbidity and organic matter hindered the inactivation performance. Singlet oxygen (1O2), hydroxyl (•OH) and organic radicals (RO•) contributed to the inactivation of E. coli, with •OH and RO• playing the prominent role. Variations of intracellular reactive oxygen species, malondialdehyde, enzymes activities, DNA contents and biochemical compositions of E. coli cells suggested that UV/PAA primarily caused oxidative damage to intracellular molecules rather than the damage to the lipids of the cell membrane, therefore effectively limited the regrowth of E. coli. Additionally, the UV/PAA process displayed an outstanding performance in disinfecting actual raw CSOs, achieving a 2.90-log inactivation of total bacteria after reaction for 4 min. These results highlighted the practical applicability and effectiveness of the UV/PAA process in the disinfection of CSOs.

3.
Environ Sci Technol ; 57(45): 17629-17639, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37906720

RESUMEN

This study provided an in-depth understanding of enhanced algae inactivation by combining ultraviolet and peracetic acid (UV/PAA) and selecting Microcystis aeruginosa as the target algae species. The electron paramagnetic resonance (EPR) tests and scavenging experiments provided direct evidence on the formed reactive species (RSs) and indicated the dominant role of RSs including singlet oxygen (1O2) and hydroxyl (HO•) and organic (RO•) radicals in algae inactivation. Based on the algae inactivation kinetic model and the determined steady-state concentration of RSs, the contribution of RSs was quantitatively assessed with the second-order rate constants for the inactivation of algae by HO•, RO•, and 1O2 of 2.67 × 109, 3.44 × 1010, and 1.72 × 109 M-1 s-1, respectively. Afterward, the coexisting bi/carbonate, acting as a shuttle, that promotes the transformation from HO• to RO• was evidenced to account for the better performance of the UV/PAA system in algae inactivation under the natural water background. Subsequently, along with the evaluation of the UV/PAA preoxidation to modify coagulation-sedimentation, the possible application of the UV/PAA process for algae removal was advanced.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Rayos Ultravioleta , Ácido Peracético/farmacología , Agua , Peróxido de Hidrógeno , Oxidación-Reducción
4.
Environ Sci Technol ; 57(28): 10478-10488, 2023 07 18.
Artículo en Inglés | MEDLINE | ID: mdl-37389809

RESUMEN

Environmental-friendly and low-cost catalysts for peracetic acid (PAA) activation are vital to promote their application for micropollutant degradation in water. In this study, powdered activated carbon (PAC) was reported to improve the degradation of sulfamethoxazole (SMX). The improvement of SMX degradation in the PAC/PAA system was expected to be because of the PAA activation rather than the co-existing H2O2 activation. Non-radical oxidation pathways, including the mediated electron-transfer process and singlet oxygen (1O2), were evidenced to play the dominant roles in the degradation of micro-organic pollutants. The graphitization of PAC, persistent free radicals, and electron-donating groups like C-OH were proposed to contribute to the activation of PAA. High SMX degradation could be achieved in the acidic and neutral conditions in the PAC/PAA system. Overall, higher dosages of PAC (0-0.02 g/L) and PAA (0-100 µM) benefited the degradation of SMX. The presence of HCO3- could lower the SMX degradation significantly, while Cl-, PO43-, and humic acid (HA) only reduced the SMX degradation efficiency a little. Overall, this study offered an efficient non-radical PAA activation method using PAC, which can be effectively used to degrade micro-organic pollutants.


Asunto(s)
Ácido Peracético , Contaminantes Químicos del Agua , Sulfametoxazol , Peróxido de Hidrógeno , Carbón Orgánico , Oxidación-Reducción
5.
J Hazard Mater ; 452: 131311, 2023 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-37030224

RESUMEN

The sulfite(S(IV))-based advanced oxidation process has attracted significant attention in removing As(III) in the water matrix for its low-cost and environmental-friendly. In this study, a cobalt-doped molybdenum disulfide (Co-MoS2) nanocatalyst was first applied to activate S(IV) for As(III) oxidation. Some parameters including initial pH, S(IV) dosage, catalyst dosage, and dissolved oxygen were investigated. The experiment results show that >Co(II) and >Mo(VI) on the catalyst surface promptly activated S(IV) in the Co-MoS2/S(IV) system, and the electron transfer between Mo, S, and Co atoms accelerated the activation. SO4•- was identified as the main active species for As(III) oxidation. Furthermore, DFT calculations confirmed that Co doping improved the MoS2 catalytic capacity. This study has proven that the material has broad application prospects through reutilization test and actual water experiments. It also provides a new idea for developing bimetallic catalysts for S(IV) activation.

6.
J Hazard Mater ; 445: 130571, 2023 03 05.
Artículo en Inglés | MEDLINE | ID: mdl-37055977

RESUMEN

In this study, Fe(Ⅱ)/peracetic acid (PAA) and Fe(Ⅱ)/sodium hypochlorite (NaClO) systems were applied as the combined preoxidation and coagulation process to enhance algae removal. A high removal rate of algae and turbidity could be achieved, with most algal cells keeping intact when adding reasonable concentrations of PAA and NaClO to enhance Fe(Ⅱ) coagulation. The variations of chlorophyll a, malondialdehyde, and intracellular reactive oxygen species suggested that moderate oxidation with only destroying surface-adsorbed organic matter rather than cell integrity was realized. The generated organic radicals, Fe(Ⅳ), and hydroxy radical played the major roles in the Fe(Ⅱ)/PAA system for the moderate oxidation of algal cells, but direct oxidation by NaClO rather than producing reactive species in the Fe(Ⅱ)/NaClO process contributed to the preoxidation. Concurrently, the in-situ formed Fe(Ⅲ) greatly promoted the agglomerating and settling of algae. The analysis of cell integrity, biochemical compositions, and fluorescence excitation-emission matrices spectra demonstrated that excess NaClO but not PAA would seriously damage the algal cells. This might be because that NaClO would directly oxidize the cell wall/membrane, while PAA mainly permeates into the cell to inactivate algae. These results suggest that Fe(Ⅱ)/PAA is an efficient strategy for algae-laden water treatment without serious algae lysis.


Asunto(s)
Hipoclorito de Sodio , Purificación del Agua , Hipoclorito de Sodio/farmacología , Hipoclorito de Sodio/química , Ácido Peracético/farmacología , Compuestos Férricos , Clorofila A , Oxidación-Reducción , Purificación del Agua/métodos , Compuestos Ferrosos/química
7.
J Hazard Mater ; 441: 129885, 2023 01 05.
Artículo en Inglés | MEDLINE | ID: mdl-36115095

RESUMEN

The hydroxylamine-enhanced Fe(II)/peracetic acid (PAA) process is a promising advanced oxidation process (AOP) with the generation of reactive species (RS) including RO•, •OH and Fe(IV). Nevertheless, it is still challenging to identify which RS is the major intermediate oxidant, and the reasons why the optimal condition is pH 4.5 rather than 3.0 are also unclear. Herein, the generation of RS and their contribution to the degradation of three micro-pollutants were explored. The quenching experiments and pseudo first-order kinetic model demonstrated that RO• rather than the other two RS were predominant. Then the overall generation and evolution pathways of RS were depicted. The elevation of pH (3.0-4.5) would accelerate the Fe(II)/Fe(III) redox cycle through the enhanced reduction of Fe(III) by hydroxylamine and induce the conversion of Fe(IV) to RO•, which benefited naproxen degradation. While the adverse Fe(III) precipitation would dominate the reduced degradation performance with the solution pH higher than 4.5. The elevation of PAA and Fe(II) dosages sped up the PAA activation, while excess hydroxylamine could consume the formed RS and exhibited an inhibitory effect. This study helps further understand the role of HA and differentiate the contribution of RS in the emerging PAA-based AOPs.


Asunto(s)
Contaminantes Ambientales , Contaminantes Químicos del Agua , Compuestos Férricos , Compuestos Ferrosos , Peróxido de Hidrógeno , Concentración de Iones de Hidrógeno , Hidroxilamina , Hidroxilaminas , Hierro , Naproxeno , Oxidantes , Oxidación-Reducción , Ácido Peracético
8.
Carbohydr Polym ; 288: 119388, 2022 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-35450649

RESUMEN

To explore effective therapeutic strategy on nonalcoholic fatty liver disease (NAFLD), the amphiphilic oligochitosan derivative containing ursodeoxycholic acid (UDCA) was synthesized and named as UBC, which could self-assemble and encapsulate exenatide (Exe) to obtain Exe-UBC nano-vesicle. Exe-UBC could be uptaken by fatty-acid cultured cells and release UDCA and Exe responsive to the high esterase concentration. In vitro experiments demonstrated that Exe-UBC activated the expression level of SIRT1 with inhibited expression of PGC-1ß and PPAR-γ and consequently exerted synergistic bioaction immediately on reducing lipidosis. After a month of Exe-UBC treated through intravenous injection, the body weight of high-fat diet feeding C57BL/6 mice recovered to ordinary level, and their lipid contents in the liver declined significantly. The recovery in hepatic function indexes like TG, AST, and ALT further revealed the superiority of Exe-UBC vesicles. These results suggested that the co-delivery of UDCA and Exe via Exe-UBC could be a potent platform for NAFLD treatment.


Asunto(s)
Enfermedad del Hígado Graso no Alcohólico , Animales , Quitosano , Dieta Alta en Grasa , Exenatida/farmacología , Hígado , Ratones , Ratones Endogámicos C57BL , Enfermedad del Hígado Graso no Alcohólico/tratamiento farmacológico , Enfermedad del Hígado Graso no Alcohólico/metabolismo , Oligosacáridos , Sirtuina 1/metabolismo , Sirtuina 1/farmacología , Sirtuina 1/uso terapéutico , Ácido Ursodesoxicólico/metabolismo , Ácido Ursodesoxicólico/farmacología , Ácido Ursodesoxicólico/uso terapéutico
9.
Water Res ; 208: 117847, 2022 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-34794020

RESUMEN

The inactivation of algae by a combined process of peracetic acid and ultraviolet irradiation (UV/PAA) was systematically investigated by choosing Microcystis aeruginosa as the reference algal species. Both hydroxyl (HO•) and organic radicals (RO•) contributed to the cell integrity loss and RO• played the dominant roles. The algae inactivation kinetics can be well fitted by the typical Hom model, showing that the inactivation kinetic curves followed a type of shoulder and exponential reduction. The initial shoulder might be induced by the protection from the cell wall. Although the results from the cell morphology, UV-vis spectra and fluorescence excitation-emission matrices analysis suggested the cell lysis and the release of algal organic matter (AOM) in the UV/PAA process, the AOM could be subsequently degraded. Humic acid (1 - 5 mg/L) inhibited the algal cell inactivation, and the presence of chloride (0.5 - 2 mM) had little effect on the cell viability reduction. However, the addition of bicarbonate (1 - 5 mM) promoted cell integrity loss. The UV/PAA process displayed better performance under the natural water background, demonstrating the extensive potential for the practical application of this approach. This study suggests that the UV/PAA process is an effective strategy for algae inactivation.


Asunto(s)
Microcystis , Purificación del Agua , Radical Hidroxilo , Ácido Peracético/farmacología , Rayos Ultravioleta
10.
Chemosphere ; 285: 131442, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34256205

RESUMEN

Degradation of tetrabromobisphenol A (TBBPA), an emerging micropollutant, by photo/Fe3+/sulfite process was investigated under different operational conditions and water matrices. 91% of TBBPA was efficiently degraded within 30 min in the Fe3+/sulfite system under sunlight irradiation when the initial pH was 6.0, which is much higher than that of TBBPA without irradiation (52%). The acceleration of radical generation and direct photolysis by photo irradiation were responsible for the enhanced TBBPA degradation. Although this process showed better performance on TBBPA degradation in weak acid conditions, the high removal efficiency was also achieved at near-neutral pH. HO, SO4- and direct photolysis contributed to TBBPA degradation. Direct photolysis and SO4- presented the dominant contribution. The degradation rate increased with elevating the Fe3+ dose (10-40 µM), but slightly decreased when the Fe3+ dose was further raised to 100 µM. Similarly, the degradation efficiency initially increased with increasing the sulfite dose (100-400 µM), but decreased when the sulfite concentration reached 1000 µM. Dissolved oxygen played a crucial role in TBBPA degradation, the presence of water matrices such as humic acid (0.8-4.0 mg/L), bicarbonate (0.5-10 mM) and chloride (0.5-10 mM) retarded TBBPA degradation. This study proposed a new efficient strategy to enhance TBBPA degradation in the Fe3+/sulfite process.


Asunto(s)
Bifenilos Polibrominados , Contaminantes Químicos del Agua , Bifenilos Polibrominados/análisis , Sulfitos , Luz Solar , Contaminantes Químicos del Agua/análisis
11.
Water Res ; 201: 117291, 2021 Aug 01.
Artículo en Inglés | MEDLINE | ID: mdl-34107364

RESUMEN

Sulfonamide antibiotics (SAs) are typical antibiotics and have attracted increasing concerns about their wide occurrence in environment as well as potential risk for human health. In this study, we applied a novel advanced oxidation process in SAs degradation by combining molybdenum sulfide and peracetic acid (MoS2/PAA). Reactive oxygen species (ROS) including HO●, CH3C(O)O●, CH3C(O)OO●, and 1O2 were generated from PAA by MoS2 activation and contributed to SAs degradation. The effects of initial pH, the dosages of PAA and MoS2, and humic acid for SAs degradation were further evaluated by selecting sulfamethoxazole (SMX) as a target SA in the MoS2/PAA process. Results suggested that the optimum pH for SMX removal was 3, where the degradation efficiency of SMX was higher than 80% after reaction for 15 min. Increasing PAA (0.075-0.45 mM) or MoS2 (0.1-0.4 g/L) dosages facilitated the SMX degradation, while the presence of humic acids retarded the SMX removal. This MoS2/PAA process also showed good efficiencies in removing other SAs including sulfaguanidine, sulfamonomethoxine and sulfamerazine. Their possible degradation pathways were proposed based on the products identification and DFT calculation, showing that apart from the oxidation of amine groups to nitro groups in SAs, MoS2/PAA induced SO2 extrusion reaction for SAs that contained six-membered heterocyclic moieties.


Asunto(s)
Ácido Peracético , Contaminantes Químicos del Agua , Antibacterianos , Disulfuros , Humanos , Peróxido de Hidrógeno , Molibdeno , Oxidación-Reducción , Sulfametoxazol , Sulfonamidas
12.
Water Res ; 189: 116605, 2021 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-33189970

RESUMEN

With the fast development of peroxymonosulfate (PMS)-dominating processes in drinking water and wastewater treatment, residual PMS is easy to come across chlorine as these processes are usually followed by secondary chlorine disinfection. The synergistic effect of PMS and chlorine on the degradation of micro-organic pollutants is investigated by selecting acetaminophen (ACT) as a reference compound for the first time in this study. Unlike conventional PMS or chlorine activation which generates reactive species such as hydroxyl radical (HO•), sulfate radical (SO4•-), chlorine radical (Cl•), and singlet oxygen (1O2), the efficient ACT removal is attributed to the direct catalytic chlorination by PMS due to the significantly enhanced consumption of chlorine along with negligible change of PMS concentration at neutral condition, and the same reaction pathways in both PMS/chlorine and chlorine processes. The kinetic study demonstrates that ACT oxidation by PMS/chlorine follows second order reaction, and the degradation efficiency can be promoted at alkaline conditions with peak rate constants at pH 9.0-10.0. The presence of chloride can enhance the removal of ACT, while ammonium and humic acid significantly retard ACT degradation. Higher formation of selected disinfection by-products (DBPs) is observed in the PMS/chlorine process than in the sole chlorination. This study highlights the important role of PMS in organic pollutants degradation and DBPs formation during the chlorination process.


Asunto(s)
Contaminantes Químicos del Agua , Purificación del Agua , Acetaminofén , Cloruros , Cloro , Desinfección , Oxidación-Reducción , Peróxidos , Contaminantes Químicos del Agua/análisis
13.
Environ Sci Pollut Res Int ; 28(4): 4342-4351, 2021 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-32944858

RESUMEN

Lanthanum molybdate/magnetite (M-La2(MoO4)3) with various LaCl3/Fe3O4 mass ratios was synthesized and optimized for selective phosphate removal from wastewater. M-La2(MoO4)3 (2:1) was selected on the basis of phosphate sorption capacity for further experiments and characterized by a variety of methods. The phosphate sorption kinetics, isotherms, and matrix effect were studied. The maximum sorption capacity at initial pH 7 indicates the possible applicability M-La2(MoO4)3 (2:1) in removing phosphate from the aquatic environment. Phosphate removal by M-La2(MoO4)3 (2:1) with high selectivity was achieved in the presence of other co-existing anions, while calcium and magnesium ions were found to inhibit the sorption process. The sorption isotherm study showed that Freundlich and Sips models fit better the Langmuir model, indicating that heterogeneous multilayer sorption was dominant during the phosphate sorption process. Sorption kinetic results showed that the pseudo-first-order kinetic model can describe well the phosphate sorption process by M-La2(MoO4)3 (2:1). Consecutive sorption-desorption runs showed that M-La2(MoO4)3 (2:1) could be reused for a few cycles. Simultaneous removal of phosphate and organic matter was achieved in real wastewater by using M-La2(MoO4)3 (2:1). The sorption mechanism was inner-sphere complexation.


Asunto(s)
Lantano , Aguas Residuales , Adsorción , Óxido Ferrosoférrico , Concentración de Iones de Hidrógeno , Cinética , Molibdeno , Fosfatos/análisis
14.
Chemosphere ; 263: 127993, 2021 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-33297033

RESUMEN

In this study, the effects of UV/chlorine pretreatment on ultrafiltration (UF) membrane fouling derived from different fractions of natural organic matter (NOM) were studied and compared. Three model organic compounds including humic acid (HA), sodium alginate (SA) and bovine serum albumin (BSA) were employed to represent different NOM fractions in natural surface water. The results suggest that membrane fouling induced from HA, SA and HA-SA-BSA mixture could be effectively mitigated by UV/chlorine pretreatment, which could be further improved by increasing the chlorine dose. Although UV irradiation alone severely aggravated BSA fouling, the addition of chlorine (0.0625 mM) to the pretreatment process could effectively avoid the fouling. The alleviation of membrane fouling is primarily ascribed to the reduction of molecular weight (MW) of organic compounds, and the decomposition of unsaturated organic species, thereby reducing the accumulation of organics on the membrane surface and pores. This is confirmed by the reduction of UV254 and fluorescent components in the feed solution and the increase of DOC in the permeate after UV/chlorine pretreatment. Membrane fouling during the filtration of untreated HA, SA, and HA-SA-BSA mixture was occupied by cake filtration and intermediate pore blocking, while UV/chlorine pretreatment led to the exacerbation of pore blocking at the initial filtration stage. The initial fouling mechanism of untreated BSA was mainly governed by complete blocking, which shifted to intermediate pore blocking after UV/chlorine pretreatment.


Asunto(s)
Ultrafiltración , Purificación del Agua , Cloro , Sustancias Húmicas , Membranas Artificiales
15.
Front Chem ; 8: 591641, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-33330378

RESUMEN

UV/persulfate (UV/PS) could effectively degrade algal cells and micro-organic pollutants. This process was firstly applied to remove Microcystis aeruginosa (M. aeruginosa) and 2,4,6-trichlorophenol (TCP) simultaneously in bench scale. Algal cells can be efficiently removed after 120 min reaction accompanied with far quicker removal of the coexisted TCP, which could be totally removed within 5 min in the UV/PS process. Both SO 4 • - and HO• were responsible for algal cells and TCP degradation, while SO 4 • - and HO• separately dominated TCP degradation and algal cells removal. Apart from the role of radicals ( SO 4 • - and HO•) for algal cells and TCP degradation, UV also played a role to some extent. Increased PS dose (0-4.5 mM) or UV intensity (2.71-7.82 mW/cm2) could enhance the performance of the UV/PS process in both TCP and algae removal. Although some intracellular organic matters can be released to the outside of algal cells due to the cell lysis, they can be further degraded by UV/PS process, which was inhibited by the presence of TCP. This study suggested the good potential of the UV/PS process in the simultaneous removal of algal cells and micro-organic pollutants.

16.
Environ Sci Technol ; 54(22): 14635-14645, 2020 11 17.
Artículo en Inglés | MEDLINE | ID: mdl-33108174

RESUMEN

Chemical oxidation using peracetic acid (PAA) can be enhanced by activation with the formation of reactive species such as organic radicals (R-O•) and HO•. Thermal activation is an alternative way for PAA activation, which was first applied to degrade micropollutants in this study. PAA is easily decomposed by heat via both radical and nonradical pathways. Our experimental results suggest that a series of reactive species including R-O•, HO•, and 1O2 can be produced through the thermal decomposition of PAA. Sulfamethoxazole (SMX), a typical sulfa drug, can be effectively removed by the thermoactivated PAA process under conditions of neutral pH. R-O• including CH3C(O)O• and CH3C(O)OO• has been shown to play a primary role in the degradation of SMX followed by direct PAA oxidation in the thermoactivated PAA process. Both higher temperature (60 °C) and higher PAA dose benefit SMX degradation, while coexisting H2O2 inhibits SMX degradation in the thermoactivated PAA process. With a variation of solution pH, conditions near a neutral value show the best performance of this process in SMX degradation. Based on the identified intermediates, transformation of SMX was proposed to undergo oxidation of the amine group and oxidative coupling reactions. This study definitively illustrates the PAA decomposition pathways at high temperature in aquatic solution and addresses the possibility of the thermoactivated PAA process for contaminant destruction, demonstrating this process to be a feasible advanced oxidation process.


Asunto(s)
Sulfametoxazol , Contaminantes Químicos del Agua , Peróxido de Hidrógeno , Oxidación-Reducción , Ácido Peracético
17.
Environ Sci Technol ; 54(1): 464-475, 2020 01 07.
Artículo en Inglés | MEDLINE | ID: mdl-31763831

RESUMEN

An advanced oxidation process of combining cobalt and peracetic acid (Co/PAA) was developed to degrade sulfamethoxazole (SMX) in this study. The formed acetylperoxy radical (CH3CO3•) through the activation of PAA by Co (Co2+) was the dominant radical responsible for SMX degradation, and acetoxyl radical (CH3CO2•) might also have played a role. The efficient redox cycle of Co3+/Co2+ allows good removal efficiency of SMX even at quite low dosage of Co (<1 µM). The presence of H2O2 in the Co/PAA process has a negative effect on the degradation of SMX due to the competition for reactive radicals. The SMX degradation in the Co/PAA process is pH dependent, and the optimum reaction pH is near-neutral. Humic acid and HCO3- can inhibit SMX degradation in the Co/PAA process, while the presence of Cl- plays a little role in the degradation of SMX in this system. Although transformation products of SMX in the Co/PAA system show higher acute toxicity, the low Co dose and SMX concentration in aquatic solution can efficiently weaken the acute toxicity. After reaction in the Co/PAA process, numerous carbon sources that could be provided for bacteria and algae growth can be produced, suggesting that the proposed Co/PAA process has good potential when combined with the biotreatment processes.


Asunto(s)
Sulfametoxazol , Contaminantes Químicos del Agua , Cobalto , Peróxido de Hidrógeno , Oxidación-Reducción , Ácido Peracético
18.
Chemosphere ; 233: 282-291, 2019 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-31176129

RESUMEN

Degradation of imipramine (IMI) in the VUV system (VUV185 + UV254) was firstly evaluated in this study. Both HO• oxidation and UV254 direct photolysis accounted for IMI degradation. The quantum yields of UV254 direct photolysis of deprotonated and protonated IMI were 1.31×10-2 and 3.31×10-3, respectively, resulting in the higher degradation efficiency of IMI at basic condition. Increasing the initial IMI concentration lowered the degradation efficiency of IMI. While elevating reaction temperature significantly improved IMI degradation efficiency through the promotion of both the quantum yields of HO• and the UV254 direct photolysis rate. The apparent activation energy was calculated to be about 26.6 kJ mol-1. Negative-linear relationships between the kobs of IMI degradation and the concentrations of HCO3-/CO32-, NOM and Cl- were obtained. The degradation pathways were proposed that cleavage of side chain and hydroxylation of iminodibenzyl and methyl groups were considered as the initial steps for IMI degradation in the VUV system. Although some high toxic intermediate products would be produced, they can be further transformed to other lower toxic products. The good degradation efficiency of IMI under realistic water matrices further suggests that the VUV system would be a good method to degrade IMI in aquatic environment.


Asunto(s)
Imipramina/química , Imipramina/toxicidad , Peróxido de Hidrógeno/química , Concentración de Iones de Hidrógeno , Hidroxilación , Oxidación-Reducción , Photobacterium/efectos de los fármacos , Fotólisis , Pruebas de Toxicidad Aguda , Rayos Ultravioleta , Vacio , Agua/química , Contaminantes Químicos del Agua/química , Contaminantes Químicos del Agua/toxicidad , Purificación del Agua/métodos
19.
Sci Total Environ ; 671: 377-387, 2019 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-30933794

RESUMEN

The magnetic poly(N-isopropylacrylamide)/chitosan hydrogel with interpenetrating network (IPN) structure was designed based on the functional groups of targeted emerging contaminants, represented by hydrophilic sulfamethoxazole (SMZ) and hydrophobic bisphenol A (BPA). The average particle size, specific surface area, and total pore volume of the hydrogel were turned out to be 103.7 µm, 60.70 m2/g and 0.0672 cm3/g, respectively. Adsorption results indicated that the maximum adsorption capacity occurred at the pH where SMZ was anionic and BPA was uncharged. When the adsorption temperature increased from 25 °C to 35 °C, the amount of adsorbed SMZ hardly changed, but that of BPA increased by two times. The adsorption capacity of the binary system (i.e., with both SMZ and BPA) was almost the same as that of the single system, indicating that simultaneous adsorption of SMZ and BPA was achieved. The adsorption equilibrium was reached quickly (within 5 min) for both SMZ and BPA. For adsorption isotherm, the Freundlich model fitted well for SMZ at 25, 35 and 45 °C. However, the adsorption of BPA exhibited the sigmoidally shaped isotherm at 25 °C with the Slips model fitting well, and both the Freundlich isotherm and the Slips isotherm fitted the data well at 35 °C and 45 °C, suggesting that the adsorption force was initially weak but greatly enhanced with an increase in adsorbate concentration or ambient temperature. The main adsorption mechanism was inferred to be electrostatic interactions for SMZ, and hydrophobic interactions as well as hydrogen bonding for BPA. The hydrogel adsorbent maintained favorable adsorption capacity for BPA after five adsorption-desorption cycles. These findings may provide a strategy for designing high performance adsorbents that can remove both hydrophilic and hydrophobic organic contaminants in the aquatic environment.

20.
Water Res ; 158: 213-226, 2019 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-31035198

RESUMEN

In this study, ultraviolet based advanced oxidation processes (UV-AOPs) including UV/persulfate (UV/PS), UV/chlorine, and UV/H2O2 were employed to alleviate ultrafiltration membrane fouling during the treatment of algae-laden water. The results show that UV/PS pretreatment exhibited the best performance on fouling control, followed by the UV/H2O2 pretreatment. The fouling mitigation performance improved with the increase of oxidant dose. However, UV/chlorine pretreatment aggravated membrane fouling, and the irreversible fouling resistance increased by five times compared with that of raw water. The dissolved organic carbon (DOC) in the algae-laden solution was reduced after UV/PS pretreatment, while either UV/chlorine or UV/H2O2 pretreatment had little influence on the DOC of feed water. UV/PS and UV/H2O2 pretreatments were effective in the degradation of fluorescent compounds, thus reducing the deposition of organic matter on the membrane surface. Additionally, the decreased concentration of hydrophobic organics, algal cells, and debris in feed water after UV/PS pretreatment was also contributed to the fouling alleviation. The aggravated irreversible fouling after UV/chlorine pretreatment was probably ascribed to the increased accumulation of hydrophobic fractions in the membrane pores. Modeling result indicates that membrane fouling during the filtration of raw algae-laden water was dominated by intermediate blocking and cake filtration mechanisms. Both UV/PS and UV/H2O2 pretreatments transformed the combined fouling mechanism into standard blocking, while UV/chlorine pretreatment aggravated the pore blocking in the initial filtration period.


Asunto(s)
Ultrafiltración , Purificación del Agua , Cloro , Peróxido de Hidrógeno , Membranas Artificiales , Agua
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