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1.
Chemosphere ; 238: 124649, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31466005

RESUMO

Electro-Fenton (EF) with peroxi-coagulation (PC) as an emerging electro-chemical advanced oxidation method has been extensively applied to treat refractory wastewater. However, the studies on the pretreatment of the raw coke plant wastewater by EF process were still lacking. In this study, a lab-scale EF system (Fe as anode and graphite as cathode) achieved the highest COD removal of 69.2% based on the preliminary experiments. The process parameters and corresponding COD removal performance were further optimized using response surface methodology (RSM) combined with Box-Behnken experimental design (BBD). The optimal conditions were obtained as: 3.2 mA cm-2 of current density, 2 h of the reaction time and 2.6 of the initial pH value, with the COD removal reaching 70.0%. Fourier infrared (FTIR), fluorescence excitation-emmission matrix (EEM) and gas chromatography-mass spectrometry (GC-MS) also revealed the degradation behaviors of dissolved organic matters (DOMs) by characterizing their structures and compositions before and after EF pretreatment, thus greatly improving the biodegradability of the wastewater. Moreover, the EF process for COD removal well followed third-order kinetics model. These findings give helpful guidance to design, optimize and control the EF process as a favourable pretreatment for actual refractory coking wastewater in practice.


Assuntos
Coque , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Purificação da Água/métodos , Peróxido de Hidrogênio/química , Cinética , Oxirredução , Eliminação de Resíduos Líquidos/normas , Poluentes Químicos da Água/química
2.
Chemosphere ; 238: 124656, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31472345

RESUMO

A composite sorbent for the simultaneous removal of both Hg2+ and SeO32- from aqueous media was produced from the solvothermal synthesis of a zirconium metal organic framework, UiO-66, in the presence of activated carbon. The composite sorbent has a large surface area of 1051 m2 g-1 with crystalized porous structures and has strong thermal stability up to 600 °C. The contaminant uptake of the sorbent follows a Langmuir adsorption isotherm with maximum sorption capacity of 205 mg g-1 and 168 mg g-1 for Hg2+ and SeO32-, respectively. Scanning electron microscopy-energy dispersive spectroscopy results show that the Se regions overlap exclusively with Zr-rich regions suggesting that SeO32- adsorption depends entirely on the exposed UiO-66 surface. In addition, X-ray photoelectron spectroscopy spectra of Se 3d and Hg 4f showed the association of SeO32- and Hg2+ on the UiO-66 and carbon surfaces, respectively. The sorbent could facilitate the development of a single process for the simultaneous removal of cationic Hg and anionic Se as well as other similar ionic metals with opposite charges from aqueous media.


Assuntos
Adsorção , Carvão Vegetal/química , Estruturas Metalorgânicas/química , Metais/isolamento & purificação , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Ânions , Cátions , Mercúrio/química , Mercúrio/isolamento & purificação , Óxidos de Selênio/isolamento & purificação , Poluentes Químicos da Água/química , Zircônio/química
3.
Chemosphere ; 238: 124665, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31473529

RESUMO

Contaminants of emerging concern (including pharmaceuticals) are not effectively removed by municipal wastewater treatment plants (WWTPs), so particular concern is related to agricultural wastewater reuse due to their possible uptake in crops irrigated with WWTPs effluents. Advanced oxidation processes (AOPs) and solar AOPs have been demonstrated to effectively remove pharmaceuticals from different aqueous matrices. In this study, an heterogeneous photocatalytic process using powdered nitrogen-doped TiO2 immobilized on polystyrene spheres (sunlight/N-TiO2) was compared to the benchmark homogenous AOP sunlight/H2O2 in a compound triangular collector reactor, to evaluate the degradation of three pharmaceuticals (carbamazepine (CBZ), diclofenac (DCF), trimethoprim (TMP)) in water. The degradation of the contaminants by sunlight and sunlight-AOPs well fit the pseudo-first order kinetic model (but for TMP under sunlight). High removal efficiency by solar photolysis was observed for DCF (up to 100%, half-life sunlight cumulative energy QS,1/2 = 2 kJ L-1, half-life time t1/2 = 32 min), while CBZ (32%, QS,1/2 = 28 kJ L-1, t1/2 = 385 min) and TMP (5% removal after 300 min) removal was poor. The degradation rate of CBZ, TMP and DCF was found to be slower during sunlight/H2O2 (QS,1/2 = 5 kJ L-1, t1/2 = 77 min; QS,1/2 = 20 kJ L-1, t1/2 = 128 min; QS,1/2 = 4 kJ L-1, t1/2 = 27 min, respectively) compared to sunlight/N-TiO2 (QS,1/2 = 4 kJ L-1, t1/2 = 55 min; QS,1/2 = 3 kJ L-1, t1/2 = 42 min; QS,1/2 = 2 kJ L-1, t1/2 = 25 min, respectively). These results are promising in terms of solar technology upscale because the faster degradation kinetics observed for sunlight/N-TiO2 process would result in smaller treatment volume, thus possibly perspective compensating the cost of the photocatalyst.


Assuntos
Carbamazepina/isolamento & purificação , Diclofenaco/isolamento & purificação , Fotólise , Luz Solar , Trimetoprima/isolamento & purificação , Cinética , Nitrogênio , Oxirredução , Fotólise/efeitos dos fármacos , Fotólise/efeitos da radiação , Titânio , Águas Residuárias/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos
4.
Chemosphere ; 239: 124765, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31520981

RESUMO

In this study, palm shell activated carbon powder (PSAC) and magnesium silicate (MgSiO3) modified PSAC (MPSAC) were thoroughly investigated for fluoride (F-) adsorption. F- adsorption isotherms showed that PSAC and MPSAC over-performed some other reported F- adsorbents with adsorption capacities of 116 mg g-1 and 150 mg g-1, respectively. Interestingly, the MgSiO3 impregnated layer changed the adsorption behavior of F- from monolayer to heterogeneous multilayer based on the Langmuir and Freundlich isotherm models verified by chi-square test (X2). Thermodynamic parameters indicated that the F- adsorption on PSAC and MPSAC was spontaneous and exothermic. PSAC and MPSAC were characterized using FESEM-EDX, XRD, FTIR and XPS to investigate the F- adsorption mechanism. Based on the regeneration tests using NaOH (0.01 M), PSAC exhibited poor regeneration (<20%) while MPSAC had steady adsorption efficiencies (∼70%) even after 5 regeneration cycles. This is due to highly polarized C-F bond was found on PSAC while Mg-F bond was distinguished on MPSAC, evidently denoting that the F- adsorption is mainly resulted from the exchange of hydroxyl (-OH) group. It was concluded that PSAC would be a potential adsorbent for in-situ F- groundwater remediation due to its capability to retain F- without leaching out in a wide range pH. MPSAC would be an alternative adsorbent for ex-situ F- water remediation because it can easily regenerate with NaOH solution. With the excellent F- adsorption properties, both PSAC and MPSAC offer as promising adsorbents for F- remediation in the aqueous phase.


Assuntos
Carvão Vegetal/química , Fluoretos/isolamento & purificação , Silicatos de Magnésio/química , Poluentes Químicos da Água/isolamento & purificação , Adsorção , Fluoretos/química , Concentração de Íons de Hidrogênio , Cinética , Microscopia Eletrônica de Varredura , Phoeniceae , Espectroscopia Fotoeletrônica , Espectroscopia de Infravermelho com Transformada de Fourier , Termodinâmica , Resíduos , Poluentes Químicos da Água/química , Purificação da Água/métodos , Difração de Raios X
5.
Chemosphere ; 238: 124648, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524610

RESUMO

Deoxynivalenol (DON) is one of the most globally prevalent mycotoxins mainly produced by Fusarium species. It can cause pollution to water environmental quality due to its water solubility. Therefore, it is necessary to develop a green and efficient detoxification technology for DON. More importantly, the toxicity of the degradation products should be assessed. Photocatalytic degradation technology has attracted increasing attention in the field of pollutants treatment, especially for wastewater treatment. Herein, the as-prepared NaYF4:Yb,Tm@TiO2 composite (UCNP@TiO2) was employed as a novel photocatalyst for the NIR-enhanced photocatalytic degradation of DON. Three intermediate products were identified by using the ESI/MS analysis and secondary mass spectrogram, with the m/z values of 329.399, 311.243 and 280.913, respectively. Furthermore, the in vitro safety of the product mixtures with various degradation time (30 min, 60 min, 90 min and 120 min) were evaluated through the influences on cell viability, cell morphology, cell cycle, intracellular reactive oxygen species (ROS) level, cell apoptosis and antioxidant capacity of HepG2 cells. There were no significant differences in these investigated indicators between the control (free of DON) and 120 min products treatment. Overall, the results indicated that the toxicity of degradation products after 120 min irradiation was much lower and even nontoxic than that of DON.


Assuntos
Micotoxinas/química , Titânio/química , Tricotecenos/química , Purificação da Água/métodos , Sobrevivência Celular/efeitos dos fármacos , Células Hep G2/citologia , Células Hep G2/efeitos dos fármacos , Células Hep G2/metabolismo , Humanos , Micotoxinas/análise , Nanopartículas/química , Espécies Reativas de Oxigênio/metabolismo , Tricotecenos/toxicidade , Águas Residuárias/análise , Águas Residuárias/química , Poluentes da Água/química
6.
Chemosphere ; 238: 124659, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524612

RESUMO

A hybrid system was developed in this study consisting of different coagulation systems and ultrafiltration (UF). Property and effect of flocs formed in different coagulation systems on ultrafiltration membrane fouling control were investigated. All three coagulation systems, as pretreatment of UF, were effective in improving membrane flux and reducing membrane resistance within an appropriate range of natural organic matters (NOM) concentration. At high initial NOM concentration, the performance of polyaluminum chloride (PAC) on NOM removal and fouling control was severely limited. For PAC-poly dimethyl diallyl ammonium chloride (PAC-PolyDMDAAC) coagulation system, the limitation of initial NOM concentration on removing NOM and alleviating membrane fouling was slightly weakened, indicating composite flocculant PAC-PolyDMDAAC produced larger flocs through combined action of charge neutralization and adsorption bridging. In PAC + PolyDMDAAC dual coagulation system, the combined action of adsorption-bridging effect, sweeping effect, and charge neutralization were the mechanisms under both low and high initial NOM concentration. Although the flocs formed in PAC + PolyDMDAAC dual coagulation system had poor recovery ability compared with those formed in PAC and PAC-PolyDMDAAC coagulation system, flocs formed through adsorption-bridging and sweeping had large size and higher ability to resist shear force, resulting in the formation of cake layer with porous and fluffy structure and less blockage in membrane pore in PAC + PolyDMDAAC dual coagulation system. These results demonstrated that dual coagulation system combined PAC coagulation and PolyDMDAAC flocculation as a pretreatment of UF process can improve the characteristics of flocs and structure of cake layer for improving NOM removal and controlling membrane fouling.


Assuntos
Hidróxido de Alumínio , Membranas Artificiais , Ultrafiltração/métodos , Adsorção , Floculação , Ultrafiltração/instrumentação , Purificação da Água/métodos
7.
Chemosphere ; 238: 124669, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524613

RESUMO

Sugar production is a water intensive process that produces a large amount of wastewaters with high concentration of chemical oxygen demand (COD), mostly consists of organic carbon compounds. Conventional treatment methods are limited to provide the necessary treatment of effluent COD to meet the regulatory limits prior to discharge. The treatment performance of electrooxidation (EO) and electrochemical peroxidation (ECP) for organic removal were investigated in a laboratory scale study. The experimental conditions were optimized for both EO and ECP using Box-Behnken Design (BBD) and the models provided highly significant quadratic models for both treatment methods. The effects of pH, H2O2 dosage, current density, and operation time were investigated using BBD. The results showed that EO could remove 75% of organics at optimum conditions of pH 5.3; current density of 48.5 mA cm-2; and operation time of 393 min. The predicted values were in reasonable agreement with measured values. ECP could remove total and soluble COD and total and dissolved organic carbon by 65, 64, 66, and 63%, respectively at optimum conditions of H2O2 dosage of 21 mL L-1; current density of 48 mA cm-2; and operation time of 361 min. The methods were compared based on removal efficiency and energy consumption during operation.


Assuntos
Beta vulgaris/química , Técnicas Eletroquímicas/métodos , Eliminação de Resíduos Líquidos/métodos , Águas Residuárias/química , Purificação da Água/métodos , Análise da Demanda Biológica de Oxigênio , Técnicas Eletroquímicas/normas , Peróxido de Hidrogênio , Indústrias , Compostos Orgânicos , Oxirredução , Açúcares , Eliminação de Resíduos Líquidos/normas , Poluentes Químicos da Água/química , Purificação da Água/normas
8.
Chemosphere ; 238: 124658, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31548174

RESUMO

Adsorption is a common process used to remove pharmaceuticals, personal care products and endocrine disrupting chemicals (PPCPs/EDCs) from water. However, as PPCPs/EDCs cover a wide range of molecules and chemical structures, prediction of the adsorption capacity is very challenging. In this study, a novel model was developed to predict adsorption isotherms of PPCPs/EDCs onto various types of adsorbents using a combination of Polanyi potential theory, molecular connectivity indices (MCIs) and molecular characteristics. Polanyi theory provided the basic mathematical form for the correlation. MCIs, hydrophobicity and H-bond count were used to normalize the Polanyi equation based on the molecular structure and interactions among the chemicals, the adsorbents, and the solution. In total, adsorption data were collected from 158 reports for 55 PPCPs/EDCs onto 306 different adsorbent materials. The correlation was first trained with 46 PPCPs/EDCs adsorbed onto 162 carbonaceous adsorbents (CAs), with 44.8% SDEV. Then the model was employed to predict 46 PPCPs/EDCs onto 118 other CAs and 9 new PPCPs/EDCs onto 23 CAs in ultrapure water, with error from 42 to 48% SDEV. When applying to non-carbonaceous adsorbents, the models can still predict the adsorption of PPCPs/EDCs with 90.09% SDEV. For the first time, a model, the PD - MCI - hydrophobic - H bond model, was developed to predict adsorption of a wide group of complicated PPCPs/EDCs onto a big variety of carbonaceous and non-carbonaceous adsorbents. The proposed model approach may provide a simple means for predicting adsorption capacities of PPCPs/EDCs onto various adsorbents.


Assuntos
Cosméticos/isolamento & purificação , Disruptores Endócrinos/isolamento & purificação , Preparações Farmacêuticas/isolamento & purificação , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água/métodos , Adsorção , Disruptores Endócrinos/análise , Interações Hidrofóbicas e Hidrofílicas , Água/química , Poluentes Químicos da Água/análise
9.
Chemosphere ; 240: 124761, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31546190

RESUMO

The formation and control of haloacetamides (HAcAms) in drinking water have raised high attention due to their high genotoxicity and cytotoxicity, especially the most cytotoxic one, diiodoacetamide (DIAcAm). In this study, the degradation of DIAcAm by UV/chlorination was investigated in terms of degradation kinetics, efficiency, influencing factors, oxidation products and toxicity evaluation. Results revealed that the degradation of DIAcAm by UV/chlorine process followed pseudo-first-order kinetics, and the rate constant between DIAcAm and OH radicals was determined as 2.8 × 109 M-1 s-1. The contribution of Cl to DIAcAm degradation by UV/chlorine oxidation was negligible. Increasing chlorine dosage and decreasing pH significantly promoted the DIAcAm degradation during UV/chlorine oxidation, but the presence of bicarbonate (HCO3-) and natural organic matter (NOM) inhibited it. The mass balance analysis of iodine species was also evaluated during UV/chlorine oxidation of DIAcAm. In this process, with DIAcAm decreasing from 16.0 to 0.8 µM-I in 20 min, IO3-, I- and HOI/I2 increased from 0 to 6.3, 6.1 and 0.5 µM-I, respectively. The increase of CHO cell viability during DIAcAm degradation indicated that the toxicity of DIAcAm could be decreased by chlorination, UV irradiation and UV/chlorine oxidation treatments, in which UV/chlorine oxidation was more effective on toxicity reduction than chlorination and UV irradiation alone.


Assuntos
Acetamidas/química , Poluentes Químicos da Água/química , Cloro/análise , Halogenação , Cinética , Oxirredução , Raios Ultravioleta , Água , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/toxicidade , Purificação da Água/métodos
10.
Chemosphere ; 238: 124583, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31425865

RESUMO

The presence of bromide (Br-) in water results in the formation of brominated disinfection byproducts (DBPs) after chlorination, which are much more cytotoxic and genotoxic than their chlorinated analogs. Given that conventional water treatment processes (e.g., coagulation, flocculation, and sedimentation) fail to remove Br- effectively, in this study, we systematically tested and compared the performance of different anion exchange resins, particularly two novel Br-selective resins, for the removal of Br-. The resins performance was evaluated under both typical and challenging background water conditions by varying the concentrations of anions and organic matter. The overall Br- removal results followed the trend of Purolite-Br ≥ MIEX-Br > IRA910 ≥ IRA900 > MIEX-Gold > MIEX-DOC. Further evaluation of Purolite-Br resin showed Br- removal efficiencies of 93.5 ±â€¯4.5% for the initial Br- concentration of 0.25 mg/L in the presence of competing anions (i.e., Cl-, NO3-, NO2-, SO42-, PO43-, and a mixture of all five), alkalinity and organic matter. In addition, experiments under challenging background water conditions confirmed the selectivity of the resins (i.e. Purolite-Br and MIEX-Br) in removing Br-, with SO42- and Cl- exhibiting the greatest influence upon the resin performance followed by NOM concentration, regardless of the NOM characteristic. After Br- removal, both the subsequent formation of brominated DBPs (trihalomethanes, haloacetic acids, and haloacetonitriles), and the total organic halogens (TOX), decreased by ∼90% under the uniform formation conditions. Overall, Br-selective resins represent a promising alternative for the efficient control of Br-DBPs in water treatment plants.


Assuntos
Resinas de Troca de Ânions/química , Brometos/análise , Trialometanos/análise , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Desinfecção/métodos , Floculação , Halogenação , Troca Iônica
11.
Chemosphere ; 238: 124575, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31446274

RESUMO

Significance of surface and ground water contamination by synthetic organic compounds has been pointed out in a very high number of papers worldwide, as well as the need of application of treatment technologies capable to assure their complete removal. Among these processes, the electrochemical advanced oxidation is an interesting option, especially when irradiated with UVC light (photo-electrochemical, P-EC) to promote homolysis of electrogenerated oxidants. In this work, the herbicide glyphosate (GLP) was used as model compound and it was electrochemically treated under UVC irradiation in the presence of NaCl and using a DSA® and BDD anodes. Total organic carbon concentration was measured throughout the electrolysis, as well as the concentration of short chain carboxylic acids and inorganic ions (NO3-, PO43-,ClO-, ClO3- and ClO4-). The synergism of the P-EC was more pronounced when using a DSA® electrode, which led to complete GLP mineralization in 1 h (0.52 A h L-1), as also confirmed by the stoichiometric formation of NO3- and PO43- ions, with an energy consumption as low as 1.25 kW h g-1. Unexpectedly, the concentration evolution of oxyhalides for the P-EC process using both anodes, especially for DSA® at 10 mA cm-2, showed the production of ClO3-, whereas detection of ClO4- species was only found when using BDD at 100 mA cm-2 for the electrochemical process. Finally, small amounts of carboxylic acids were detected, including dichloroacetic acid, especially when using a BDD electrode.


Assuntos
Técnicas Eletroquímicas/métodos , Glicina/análogos & derivados , Água Subterrânea/química , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/química , Purificação da Água/métodos , Ácidos Carboxílicos/análise , Diamante/química , Eletrodos , Glicina/análise , Oxidantes/química , Oxirredução , Raios Ultravioleta
12.
Chemosphere ; 238: 124633, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31454747

RESUMO

Three different source waters were investigated using virgin and pre-used anion exchange resins, coagulation, and ion exchange combined with coagulation (IEX&Coagulation). The hydrophobicity, size distribution and charge of natural organic matter (NOM) were used to evaluate its removal. Dissolved organic carbon (DOC) removal by pre-used IEX resin was 67-79%. A consistent ratio of different hydrophobicity fractions was found in the removed DOC, while the proportion and quantity of the molecular weight fraction around 1 kDa was important in understanding the treatability of water. For pre-used resin, organic compounds were hypothesised to be restricted to easily accessible exchange sites. Comparatively, virgin resin achieved higher DOC removals (86-89%) as resin fouling was absent. Charge density and the proportion of the hydrophobic fraction were found to be important indicators for the specific disinfection byproduct formation potential (DBP-FP). Treatment of raw water with pre-used resin decreased the specific DBP-FP by between 2 and 43%, while the use of virgin resin resulted in a reduction of between 31 and 63%. The highest water quality was achieved when the combination of IEX and coagulation was used, reducing DOC and the specific DBP-FP well below that seen for either process alone.


Assuntos
Compostos Orgânicos/análise , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Resinas de Troca de Ânions/química , Floculação , Interações Hidrofóbicas e Hidrofílicas , Troca Iônica
13.
Chemosphere ; 238: 124625, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31466008

RESUMO

The cyanotoxin cylindrospermopsin was discovered during a drinking water-related outbreak of human poisoning in 1979. Knowledge about the degradation of cylindrospermopsin in waterbodies is limited. So far, only few cylindrospermopsin-removing bacteria have been described. Manganese-oxidizing bacteria remove a variety of organic compounds. However, this has not been assessed for cyanotoxins yet. We investigated cylindrospermopsin removal by manganese-oxidizing bacteria, isolated from natural and technical systems. Cylindrospermopsin removal was evaluated under different conditions. We analysed the correlation between the amount of oxidized manganese and the cylindrospermopsin removal, as well as the removal of cylindrospermopsin by sterile biogenic oxides. Removal rates in the range of 0.4-37.0 µg L-1 day-1 were observed. When MnCO3 was in the media Pseudomonas sp. OF001 removed ∼100% of cylindrospermopsin in 3 days, Comamonadaceae bacterium A210 removed ∼100% within 14 days, and Ideonella sp. A288 and A226 removed 65% and 80% within 28 days, respectively. In the absence of Mn2+, strain A288 did not remove cylindrospermopsin, while the other strains removed 5-16%. The amount of manganese oxidized by the strains during the experiment did not correlate with the amount of cylindrospermopsin removed. However, the mere oxidation of Mn2+ was indispensable for cylindrospermopsin removal. Cylindrospermopsin removal ranging from 0 to 24% by sterile biogenic oxides was observed. Considering the efficient removal of cylindrospermopsin by the tested strains, manganese-oxidizing bacteria might play an important role in cylindrospermopsin removal in the environment. Besides, manganese-oxidizing bacteria could be promising candidates for biotechnological applications for cylindrospermopsin removal in water treatment plants.


Assuntos
Toxinas Bacterianas/análise , Burkholderiales/metabolismo , Comamonadaceae/metabolismo , Manganês/metabolismo , Pseudomonas/metabolismo , Uracila/análogos & derivados , Purificação da Água/métodos , Água Potável/metabolismo , Compostos de Manganês/metabolismo , Oxirredução , Óxidos/metabolismo , Uracila/análise
14.
Chemosphere ; 238: 124632, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31472355

RESUMO

Fenton (Fe2+ + H2O2) reagents acting to remove organic pollutants possess dual functions, including the oxidation by hydroxyl radicals and the coagulation of Fe(III). Previous papers have extensively studied the oxidation reactions by hydroxyl radicals, however, the coagulation role of Fenton for benzoic acid (BA) removal is not clear. Comparing three coagulation systems, it was found that Fenton coagulation possesses a significant advantage for the removal of BA. Through Fenton conditional experiments, results showed that with the increase of H2O2 dosage, not only was the Fenton oxidation effect improved, but the Fenton coagulation effect was also significantly enhanced. Interestingly, the flocs produced by in situ Fenton possess a better coagulation effect than an aged Fenton system when processing BA. To further explain these results, Zeta potential, Transmission electron microscope (TEM), X-ray diffraction (XRD), X-ray absorption fine structure (EXAFS) and Brunner-Emmet-Teller (BET) measurements were used for characterization, and we found that the flocs produced by Fenton possessed a smaller particle size, lower polymerization states and a larger specific surface area and pore volume, which exposed more active sites to create a better coagulation effect. Additionally, through Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and Gas chromatography-mass spectrometer (GC-MS), we found that in situ Fenton oxidation and coagulation have synergistic effects, and the carboxyl-containing intermediates produced by the Fenton oxidation of BA can be combined with hydroxyl active sites of the flocs produced by in situ Fenton, resulting in a better removal effect. Finally, Fenton oxidation increases oxygen/carbon (O/C) to promote Fenton coagulation, and in situ Fenton more fully utilizes the active sites on the flocs' surface.


Assuntos
Ácido Benzoico/análise , Peróxido de Hidrogênio/química , Ferro/química , Esgotos/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Floculação , Radical Hidroxila/química , Oxirredução , Espectroscopia Fotoeletrônica , Difração de Raios X
15.
Chemosphere ; 238: 124675, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524615

RESUMO

A synergistic combination of chloride and copper powder was proposed as a new method to reductively remove arsenic from highly-acidic wastewater with high arsenic content (HAWA). As(III) was reduced to As(0) by copper powder in the presence of chloride and were effectively removed from HAWA. The procedure to remove arsenic was optimized as follows: initial H+ concentration of 5 mol L-1, Cu-to-As molar ratio of 8, Cl-to-As molar ratio of 10, a reaction temperature of 60 °C, copper powder particle size of 68-24 µm, and a stirring speed of 300 r min-1. Under these optimal conditions, the removal rate of arsenic was close to 100%. Kinetics results suggested that the arsenic removal process was controlled by both diffusion and chemical reactions with an apparent activation energy of 29.78 kJ mol-1. The XRD results showed that the removed arsenic in the residue existed primarily in the form of AsCu3 alloy.


Assuntos
Arsênico/análise , Águas Residuárias/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Cloretos/química , Cloro , Cobre/química , Concentração de Íons de Hidrogênio
16.
Chemosphere ; 238: 124682, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524619

RESUMO

Plant growth-promoting bacteria (PGPB) are considered a promising tool to improve biomass production and water remediation by the aquatic plant, duckweed; however, no effective methodology is available to utilize PGPB in large hydroponic systems. In this study, we proposed a two-step cultivation process, which comprised of a "colonization step" and a "mass cultivation step," and examined its efficacy in both bucket-scale and flask-scale cultivation experiments. We showed that in the outdoor bucket-scale experiments using three kinds of environmental water, plants cultured through the two-step cultivation method with the PGPB strain, Acinetobacter calcoaceticus P23, yielded 1.9 to 2.3 times more biomass than the control (without PGPB inoculation). The greater nitrogen and phosphorus removals compared to control were also attained, indicating that this strategy is useful for accelerating nutrient removal by duckweed. Flask-scale experiments using non-sterile pond water revealed that inoculation of strain P23 altered duckweed surface microbial community structures, and the beneficial effects of the inoculated strain P23 could last for 5-10 d. The loss of the duckweed growth-promoting effect was noticeable when the colonization of strain P23 decreased in the plant. These observations suggest that the stable colonization of the plant with PGPB is the key for maintaining the accelerated duckweed growth and nutrient removal in this cultivation method. Overall, our results suggest the possibility of an improved duckweed production using a two-step cultivation process with PGPB.


Assuntos
Acinetobacter calcoaceticus/metabolismo , Araceae/crescimento & desenvolvimento , Araceae/microbiologia , Hidroponia/métodos , Microbiota/fisiologia , Biomassa , Água Doce , Nitrogênio/análise , Nutrientes , Fósforo/análise , Desenvolvimento Vegetal , Purificação da Água/métodos
17.
Chemosphere ; 238: 124687, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524622

RESUMO

The development of highly efficient and green catalytic oxidation process based on peroxymonosulfate (PMS) activation has been identified to be a significant yet challenging objective in the environmental catalysis field. A simple, environmentally benign and highly effective catalytic oxidation system was innovatively constructed by coupling NaBO2 and PMS for the removal of Acid Red 1. The catalytic mechanism in the NaBO2/PMS system was elucidated by electron paramagnetic resonance (EPR) combined with several radical capture reagents (ascorbic acid, methanol, tert-butyl alcohol, ethanol and l-histidine). The experimental results indicated that singlet oxygen (1O2) severed as the predominant reactive oxygen species (ROS) rather than the HO or during the catalytic oxidation process, at variance with the reported radical pathway in the Co2+/PMS system. Inspiringly, p-benzoquinone (p-BQ) as a trapping agent in most advanced oxidation process could be turned into the positive one in the NaBO2/PMS system, achieving a nearly 3-times enhancement in terms of the rate constant for AR1 removal. More interestingly, sodium chloride (NaCl) presented the same enhancement effect as p-benzoquinone due to generation of hypochlorous acid (HOCl) and more 1O2, which was completely different from the reported. This study develops a highly efficient green oxidation process and opens up a new insight in the remediation of contaminated water.


Assuntos
Boratos/química , Oxirredução , Peróxidos/química , Rodaminas/análise , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Catálise , Oxigênio Singlete/metabolismo
18.
Chemosphere ; 238: 124690, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524625

RESUMO

Doxorubicin (DOX) originated from users' urine has been an emerging environmental pollutant due to its significant genotoxicity to mankind. Thus, urine source separation is a potential strategy to isolate DOX at a higher concentration and reduce the burden of downstream wastewater treatment. To develop highly efficient, easy separation and retrievable materials for individual patient to conveniently remove DOX from own urine, magnetic Cu3(PO4)2 nanoflowers were prepared through anchoring amino-functionalized magnetic nanoparticles on the Cu3(PO4)2 nanoflowers. Characterizations revealed the magnetic nanoflowers were spherical in shape with a mean size of 15 µm, and porous and hierarchical in structure. Magnetic nanoparticles located the surface of petals. Multibatch experiments were performed to assess the removal performance of DOX from aqueous solution. The magnetic nanoflowers exhibited excellent removal efficiency of DOX under weakly alkaline condition at ambient temperature. Linear and non-linear analyses were carried out to compare the best fitting kinetics and isotherms. Sorption kinetic data best fitted the pseudo-second order model. The Freundlich isotherm explained equilibrium sorption data with R2 = 0.993 higher than that for the Langmuir isotherm. When the pH of synthetic urine was adjusted to weakly alkaline (pH 8.0-9.0), over 95% of DOX (20 mg L-1) was removed by a little of magnetic nanoflowers (50 mg L-1) within 5 min. Meanwhile, the magnetic nanoflowers could be easily separated and recovered from the synthetic urine by a magnet. So, for individual urine source separation strategy, the magnetic nanoflower seems to be an efficient, convenient and inexpensive approach to remove DOX from human urine.


Assuntos
Cobre/química , Doxorrubicina/análise , Magnetismo/métodos , Urina/química , Purificação da Água/métodos , Adsorção , Humanos , Concentração de Íons de Hidrogênio , Fenômenos Magnéticos , Nanopartículas/química , Fosfatos/química , Águas Residuárias/química
19.
Chemosphere ; 238: 124691, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524626

RESUMO

In recent years, forward osmosis (FO) has represented numerous potential applications in safe water production. In this study, we improved the performance of FO thin film composite (TFC) membranes for the removal of trace organic compounds (TOrCs) by tuning the chemistry of its top active layer. The TFC membranes were synthesized by interfacial polymerization (IP) reaction between amine-containing monomers, e.g., meta-phenylene diamine (MPD) or para-phenylenediamine (PPD), and an acid chloride monomer, e.g., trimesoyl chloride (TMC). Owing to three free amine functionals over main core, melamine was used in the amine monomers solution to increase cross-linking among polyamide chains. Chemical and morphological characterization of the prepared membranes confirmed that melamine was successfully incorporated into the chemical structure of the top PA layer. Two agricultural toxic materials (atrazine and diazinon) were used to investigate the capability of the newly fabricated membranes in the removal of TOrCs. The obtained results showed that melamine-improved FO membranes provided higher atrazine and diazinon rejections in two different FO membrane configurations, including active layer facing feed solution (ALF) and active layer facing draw solution (ALD). The highest rejections of both diazinon (99.4%) and atrazine (97.3%) were achieved when the melamine modified MPD-based membrane served in ALF mode with 2 M NaCl as a draw solution.


Assuntos
Substâncias Húmicas/análise , Osmose/fisiologia , Purificação da Água/instrumentação , Purificação da Água/métodos , Atrazina/análise , Diazinon/análise , Membranas Artificiais , Nylons/química , Fenilenodiaminas/química , Polimerização , Cloreto de Sódio/química , Triazinas/química , Ácidos Tricarboxílicos/química , Água/química
20.
Chemosphere ; 238: 124693, 2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-31524627

RESUMO

In this work, self-assembled gels were prepared with exfoliated montmorillonite and chitosan (EMCG) as the adsorbent for removing methyl orange (MO) from water in absence and presence of methylene blue (MB). Several techniques including scanning electron microscope (SEM), zeta potential, fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) were used for the characterization of the EMCG before and after removal of MO. The EMCG performed well in the removal of MO attributing to the electrostatic attraction, cation exchange and hydrogen bond. The adsorption behaviors were followed pseudo-second-order and Langmuir isotherm. More surprisingly, the maximum adsorption capacity of MO was obviously enhanced in the presence of MB that it increased from 545 mg g-1 (absence of MB) to 1060 mg g-1 with the shielding effect of MB on EMCG which allowed MO and MB to alternately arrange at the adsorption sites. This finding of the synergistic effect between the two dyes on the proposed composite opens up new vistas to imagine the enhanced purification of the wastewater with multiple dyes co-existed using the multifunctional adsorbents.


Assuntos
Compostos Azo/análise , Bentonita/química , Quitosana/química , Azul de Metileno/química , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Adsorção , Compostos Azo/química , Corantes/química , Géis , Espectroscopia Fotoeletrônica , Espectroscopia de Infravermelho com Transformada de Fourier , Águas Residuárias/química , Poluentes Químicos da Água/química
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