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1.
Environ Sci Technol ; 57(15): 6063-6071, 2023 04 18.
Artigo em Inglês | MEDLINE | ID: mdl-36988440

RESUMO

Pharmaceuticals have been detected at high concentrations in municipal solid waste (MSW) landfill leachates, which are recognized as an underestimated source of pharmaceutical residues in the environment. However, limited efforts have been made to characterize pharmaceuticals in MSW landfill refuse, which is also of significant concern given the potential long-term environmental impact. Herein, we excavated landfill refuse from six cells with landfill ages of 7-27 years in the largest MSW landfill in Shanghai (in each cell, landfill refuse was collected from different depths of 2-8 m) and analyzed samples for the presence of 55 pharmaceuticals, including antibiotics and non-antibiotics. The results reveal the presence of 42 pharmaceuticals in landfill refuse, with median concentrations ranging from 0.30 to 116 µg/kg. Antibiotic and non-antibiotic pharmaceuticals exhibited diverse concentration trends with age, related to changes in policy intervention and consumption over time. Different concentration variations of individual pharmaceuticals were observed in refuse samples excavated at different depths and positively correlated to their sorption ability. The mass of pharmaceuticals in the investigated landfill was estimated from the obtained concentrations to be 80-220 tons with 95% probability, based on Monte Carlo analysis. To the best of our knowledge, this study provides the first estimate of pharmaceutical mass in an MSW landfill. The results will be helpful for understanding the potential long-term environmental impact of pharmaceuticals in landfills.


Assuntos
Eliminação de Resíduos , Resíduos Sólidos , Eliminação de Resíduos/métodos , China , Antibacterianos , Instalações de Eliminação de Resíduos , Preparações Farmacêuticas
2.
J Org Chem ; 86(2): 1591-1600, 2021 01 15.
Artigo em Inglês | MEDLINE | ID: mdl-33372521

RESUMO

A practical and efficient method for the synthesis of α-fluorothioacrylamide was developed from selective defluorinative sulfuration of trifluoropropanamides with disulfides. The N-chelation-assisted copper-catalyzed defluorination and sulfurization reactions feature excellent functional group tolerance and incorporation of both sulfur atoms of disulfides into acrylamides.

3.
Environ Sci Technol ; 55(8): 4822-4830, 2021 04 20.
Artigo em Inglês | MEDLINE | ID: mdl-33792295

RESUMO

Unused or expired pharmaceutical and personal care products (PPCPs) are usually discharged into municipal solid wastes, then travel to landfills, and eventually percolate into leachates. However, knowledge of their occurrence and temporal dynamics in leachates is limited, making landfill leachate an underappreciated emission source of PPCPs. Furthermore, the differences in PPCP variations in landfill leachates emphasize the necessity for identifying the influencing factors and elucidating the mechanisms for PPCP fluctuations. In this study, successive monthly monitoring of PPCPs in leachates throughout an entire year was performed to determine their seasonal variations and identify their influencing factors. Furthermore, five pairs of additional sampling campaigns were conducted before and after rainfall events during wet seasons to elucidate the influencing mechanisms. The results showed that there was a distinct seasonal variation in PPCPs in landfill leachates-elevated levels during the wet period (from April to September, with a mean concentration of 17.0 µg/L for total monitored PPCPs)-when compared to other months (mean concentration of 3.8 µg/L). Rainfall played a considerable role in mediating PPCP concentrations in leachates. The PPCP responses to five rainfall episodes further verified the influence of rainfall and demonstrated that the tendency to PPCP concentration increase was related to rainfall precipitation. Torrential rain events (i.e., 24 h cumulative precipitation of 50-99.9 mm) led to the most significant increases in PPCP concentrations in landfill leachates. In addition, the hydrophilicity of PPCPs contributed to the different fluctuations during the 1 year investigation and different responses to rainfall. To the best of our knowledge, this study provides the first direct evidence supporting the influence of rainfall on PPCPs in landfill leachates, which can help better understand the occurrence and behavior of emerging contaminants in this underappreciated emission source.


Assuntos
Cosméticos , Preparações Farmacêuticas , Poluentes Químicos da Água , Estações do Ano , Instalações de Eliminação de Resíduos , Poluentes Químicos da Água/análise
4.
Environ Sci Technol ; 54(16): 9757-9768, 2020 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-32560585

RESUMO

Pharmaceutical and personal care products (PPCPs) have been the focus of increasing concern in recent decades due to their ubiquity in the environment and potential risks. Out-of-date PPCPs are usually discharged into municipal solid wastes (MSWs), enter the leachates in MSW landfills, and have serious adverse effects on the surrounding water environment. However, the occurrence and removal of PPCPs from landfill leachates have rarely been examined to date. This lack of knowledge makes the landfill an underestimated source of PPCPs in the environment. In this review, we collected the relevant publications of PPCPs in landfill leachates, systematically summarized the occurrence of PPCPs in landfill leachates globally, evaluated the removal performances for various PPCPs by different types of on-site full-scale leachate treatment processes, and assessed the impacts of landfill leachates on PPCPs in the adjacent groundwater. In particular, influencing factors for PPCPs in landfill leachates, including the physicochemical properties of PPCPs, climate conditions, and characteristics of landfill sites (i.e., landfill ages) as well as sociological factors (i.e., economic development), were extensively discussed to understand their occurrence patterns. Future perspectives were also proposed in light of the identified knowledge gaps. To the best of our knowledge, this is the first review regarding the occurrence and removal of PPCPs from landfill leachates worldwide.


Assuntos
Cosméticos , Água Subterrânea , Preparações Farmacêuticas , Eliminação de Resíduos , Poluentes Químicos da Água , Cosméticos/análise , Resíduos Sólidos , Instalações de Eliminação de Resíduos , Poluentes Químicos da Água/análise
5.
Water Sci Technol ; 82(5): 998-1008, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-33031076

RESUMO

The feasibility of an advanced oxidation process based upon sodium persulfate (SPS) activated simultaneously by heat (50 °C) and nanoscale zero-valent iron (nZVI) on benzene removal was investigated. The experimental results strongly showed the synergistic effect of thermal and nZVI activation to SPS and benzene removal was enhanced with the increase of SPS/nZVI/benzene molar ratio. Specifically, 94% of benzene could be removed in 1 hr at 50 °C at the SPS/nZVI/benzene molar ratio of 10/5/1. The radical scavenger tests and electron paramagnetic resonance (EPR) analysis confirmed that SO4•- was the predominant species contributing to benzene degradation. Further, the effects of the solution matrix on benzene elimination were investigated. The results indicated that benzene destruction in the thermally activated SPS/nZVI system performed better under acidic conditions, and the high concentration of both Cl- and HCO3 - had adverse effects on benzene elimination. The test for the performance of benzene degradation in the actual groundwater demonstrated that benzene could be degraded entirely at SPS/nZVI/benzene molar ratio of 40/40/1 at 50 °C, indicating that the synergistic catalysis of thermal and nZVI activation to SPS is exploitable and the thermally activated SPS/nZVI system can be applicable to the remediation of benzene contaminated groundwater.


Assuntos
Água Subterrânea , Poluentes Químicos da Água , Benzeno , Ferro , Oxirredução , Poluentes Químicos da Água/análise
6.
Chem Eng J ; 362: 243-250, 2019 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-31588180

RESUMO

This study investigated the reductive initiation for the depletion of highly oxidized/perhalogenated pollutants, specifically the degradation of carbon tetrachloride (CT) was induced by adding methanol (MeOH) into a ferrous ion (Fe(II)) activated calcium peroxide (CaO2) system. The results indicated that CT could be completely degraded within 20 min at CaO2/Fe(II)/MeOH/CT molar ratio of 30/40/10/1 in this system. Scavenging tests suggested that both superoxide radical anion (O2 •-) and carbon dioxide radical anion (CO2 •-) were predominant reactive species responsible for CT destruction. Hydroxymethyl radicals (•CH2OH), an intermediate in the transformation of MeOH, could also initiate CT degradation by reducing C-Cl bond. GC/MS analysis identified CHCl3, C2Cl4, and C2Cl6 as the intermediates accompanied by CT destruction, and a reduction mechanism for CT degradation was proposed accordingly. In addition, the impact of solution matrix and initial solution pH were evaluated, and the results showed that Cl-, NO3 -, and HCO3 - had adverse effects on CT degradation. Moreover, the alkaline condition was unfavorable to CT depletion. In conclusion, the results obtained in the actual groundwater tests encouragingly demonstrated that the CaO2/Fe(II)/MeOH process is a highly promising technique for the remediation of CT-contaminated groundwater.

7.
Chem Eng J ; 361: 919-928, 2019 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-32095103

RESUMO

This study conducted a comparison of the CaO2-based Fenton (CaO2/Fe(II)) and Fenton-like (CaO2/Fe(III)) systems on their benzene degradation performance. The H2O2, Fe(II), Fe(III), and HO● variations were investigated during the benzene degradation. Although benzene has been totally removed in the two systems, the variation patterns of the investigated parameters were different, leading to the different benzene degradation patterns. In terms of the Fe(II)/Fe(III) conversion, the CaO2/Fe(II) and CaO2/Fe(III) systems were actually inseparable and had the inherent mechanism relationships. For the CaO2/Fe(III) system, the initial Fe(III) must be converted to Fe(II), and then the consequent Fenton reaction could be later developed with the regenerated Fe(II). Moreover, some benzene degradation intermediates could have the ability to facilitate the transformation of the Fe(III) to Fe(II) without the classic H2O2-associated propagation reactions. By varying the Fe(II) dosing method, an effective degradation strategy has been developed to take advantage of the two CaO2-based oxidation systems. The proposed strategy was further successfully tested in TCE degradation, therefore extending the potential for the application of this technique.

8.
Sep Purif Technol ; 226: 13-21, 2019 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-31933532

RESUMO

In this study, nCaO2 was synthesized successfully and applied in the Fe(II)-based catalytic environments in investigating trichloroethylene (TCE) removal performance. nCaO2 with the particle sizes in the range of 50-200 nm was prepared, and it performed better for TCE removal when compared to the conventional CaO2. Further experimental results showed that 70.4% of TCE could be removed in 180 min at the nCaO2/Fe(II)/TCE molar ratio of 1/2/1, while this data was elevated to 86.1% in the presence of citric acid (CA) at the nCaO2/Fe(II)/CA/TCE molar ratio of 1/2/2/1 in the same test period. Probe compound tests, specifically designed for free radicals confirmation, demonstrated the presence of HO• and O2 -•. Moreover, scavenging tests indicated that HO• was the major radical responsible for TCE degradation but O2 -• promoted the removal of TCE in both nCaO2/Fe(II) and nCaO2/Fe(II)-CA system. In addition, the effects of initial solution pH and anions (Cl-, HCO3 -) were also evaluated. The performance of TCE degradation in actual groundwater demonstrated that both nCaO2/Fe(II) and nCaO2/Fe(II)-CA systems can be applicable for TCE removal in ISCO practice and the nCaO2/Fe(II)-CA system is much promising technique. These fundamental data strongly confirmed the feasibility and potential of nCaO2 based technique in the remediation of TCE contaminated groundwater.

9.
Purinergic Signal ; 14(3): 285-298, 2018 09.
Artigo em Inglês | MEDLINE | ID: mdl-29974392

RESUMO

With immunohistochemical and Western blot techniques, P2X1 receptors were detected in the whole mouse gastrointestinal tract and pancreatic islets of mouse and human. (1) δ Cells containing somatostatin (SOM) in the stomach corpus, small intestines, distal colon, pancreatic islets of both mouse and human express P2X1 receptors; (2) strong immunofluorescence of P2X1 receptors was detected in smooth muscle fibers and capillary networks of the villus core of mouse intestine; and (3) P2X1 receptor-immunoreactive neurons were also detected widely in both mouse myenteric and submucosal plexuses, all of which express SOM. The present data implies that ATP via P2X1 receptors is involved in SOM release from pancreatic δ cells, enteric neurons, and capillary networks in villi.


Assuntos
Trato Gastrointestinal/metabolismo , Ilhotas Pancreáticas/metabolismo , Receptores Purinérgicos P2X1/metabolismo , Células Secretoras de Somatostatina/metabolismo , Animais , Trato Gastrointestinal/citologia , Humanos , Ilhotas Pancreáticas/citologia , Camundongos , Plexo Mientérico/citologia , Plexo Mientérico/metabolismo , Células Secretoras de Somatostatina/citologia
10.
Chem Eng J ; 353: 657-665, 2018 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-31467481

RESUMO

Calcium peroxide (CaO2) is a stable hydrogen peroxide (H2O2) carrier, and the CaO2/Fe(II) system has been applied for treatment of various pollutants. It is commonly reported in the literature that hydroxyl radical (HO●) and superoxide radical anions (O2 ●-) are the two main reactive oxygen species (ROSs) generated in the CaO2/Fe(II) system. However, many of the reported results were deduced from degradation performance rather than specific testing of radical generation. Thus, the specific generation of ROSs and the influence of system conditions on ROSs yield is still unclear. To our knowledge, this is the first study specifically focusing on the generation of HO● and O2 ●- in the CaO2/Fe(II) system. Experimental conditions were optimized to investigate the production of HO● and O2 ●-. The results showed the influences of CaO2, Fe(II), and solution pH on HO● and O2 ●- generation, and the HO● generation efficiency was reported for the first time. In addition, the ROSs generation pathways in the CaO2/Fe(II) system were elucidated. A strategy for enhancing HO● yield is developed, based on the continuously dosing Fe(II). This proposed strategy has implications for the effective application of in situ chemical oxidation employing CaO2/Fe(II) for groundwater remediation.

11.
Purinergic Signal ; 13(4): 529-544, 2017 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-28823092

RESUMO

Traumatic brain injury (TBI) is the leading cause of death and disability for people under the age of 45 years worldwide. Neuropathology after TBI is the result of both the immediate impact injury and secondary injury mechanisms. Secondary injury is the result of cascade events, including glutamate excitotoxicity, calcium overloading, free radical generation, and neuroinflammation, ultimately leading to brain cell death. In this study, the P2X7 receptor (P2X7R) was detected predominately in microglia of the cerebral cortex and was up-regulated on microglial cells after TBI. The microglia transformed into amoeba-like and discharged many microvesicle (MV)-like particles in the injured and adjacent regions. A P2X7R antagonist (A804598) and an immune inhibitor (FTY720) reduced significantly the number of MV-like particles in the injured/adjacent regions and in cerebrospinal fluid, reduced the number of neurons undergoing apoptotic cell death, and increased the survival of neurons in the cerebral cortex injured and adjacent regions. Blockade of the P2X7R and FTY720 reduced interleukin-1ßexpression, P38 phosphorylation, and glial activation in the cerebral cortex and improved neurobehavioral outcomes after TBI. These data indicate that MV-like particles discharged by microglia after TBI may be involved in the development of local inflammation and secondary nerve cell injury.


Assuntos
Lesões Encefálicas Traumáticas/patologia , Guanidinas/farmacologia , Microglia/patologia , Antagonistas do Receptor Purinérgico P2X/farmacologia , Quinolinas/farmacologia , Receptores Purinérgicos P2X7/metabolismo , Animais , Lesões Encefálicas Traumáticas/metabolismo , Micropartículas Derivadas de Células/patologia , Masculino , Microglia/efeitos dos fármacos , Distribuição Aleatória , Ratos , Ratos Sprague-Dawley
12.
Environ Sci Technol ; 51(4): 2262-2270, 2017 02 21.
Artigo em Inglês | MEDLINE | ID: mdl-28118709

RESUMO

Bezafibrate (BF), a frequently detected pharmaceutical in the aquatic environment, could be effectively removed by ozonation. However, the toxicity of treated water increased, suggesting the generation of toxic oxidation products (OPs). In this study, eight OPs of BF ozonation were identified using a LTQ Orbitrap hybrid mass spectrometer coupled with HPLC, and six of them have not been previously reported during BF ozonation. Based on the abundant fragments and high assurance of accurate molar mass, structure elucidation was comprehensively performed and discussed. Hydroxylation, loss of methyl propionic acid group, and Crigée mechanism were observed as the oxidation mechanisms of BF ozonation. The toxicity of identified OPs calculated by quantitative structure activity relationship indicated that three OPs were probably more toxic than the precursor compound BF. This result together with the evolution of identified OPs in the treated solutions, indicated that two OPs, namely N-(3,4-dihydroxyphenethyl)-4-chlorobenzamide and N-(2,4-dihydroxyphenethyl)-4-chlorobenzamide, were the potential toxicity-causing OPs during BF ozonation. To the best of our knowledge, this is the first attempt to identify toxicity-causing OPs during the BF ozonation.


Assuntos
Bezafibrato , Purificação da Água , Oxirredução , Ozônio/química , Poluentes Químicos da Água/química
13.
Chem Eng J ; 325: 188-198, 2017 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-29104449

RESUMO

The enhancement effect of an environmentally friendly reducing agent, ascorbic acid (AA), on trichloroethene (TCE) degradation by Fe(III)-activated calcium peroxide (CP) was evaluated. The addition of AA accelerated the transformation of Fe(III) to Fe(II), and the complexation of Fe(III)/Fe(II) with AA and its products alleviated the precipitation of dissolved iron. These impacts enhanced the generation of reactive oxygen species (ROSs). Investigation of ROSs using chemical probe tests, electron paramagnetic resonance (EPR) tests, and radical scavenger tests strongly confirm large production of hydroxyl radicals (HO•) that is responsible for TCE degradation. The generation of Cl- from the degraded TCE was complete in the enhanced CP/Fe(III)/AA system. The investigation of solution matrix effects showed that the TCE degradation rate decreases with the increase in solution pH, while Cl-, SO42- and NO3- anions have minor impact. Conversely, HCO3- significantly inhibited TCE degradation due to pH elevation and HO• scavenging. The results of experiments performed using actual groundwater indicated that an increase in reagent doses are required for effective TCE removal. In summary, the potential effectiveness of the CP/Fe(III)/AA oxidation system for remediation of TCE contaminated groundwater has been demonstrated. Additional research is needed to develop the system for practical implementation.

14.
Chem Eng J ; 309: 22-29, 2017 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-28959136

RESUMO

Complete degradation of benzene by the Fe(III)-activated sodium percarbonate (SPC) system is demonstrated. Removal of benzene at 1.0 mM was seen within 160 min, depending on the molar ratios of SPC to Fe(III). A mechanism of benzene degradation was elaborated by free-radical probe-compound tests, free-radical scavengers tests, electron paramagnetic resonance (EPR) analysis, and determination of Fe(II) and H2O2 concentrations. The degradation products were also identified using gas chromatography-mass spectrometry method. The hydroxyl radical (HO.) was the leading species in charge of benzene degradation. The formation of HO. was strongly dependent on the generation of the organic compound radical (R.) and superoxide anion radical (O.). Benzene degradation products included hydroxylated derivatives of benzene (phenol, hydroquinone, benzoquinone, and catechol) and aliphatic acids (oxalic and fumaric acids). The proposed degradation pathways are consistent with radical formation and identified products. The investigation of selected matrix constituents showed that the Cl and HCO3 had inhibitory effects on benzene degradation. Natural organic matter (NOM) had accelerating influence in degrading benzene. The developed system was tested with groundwater samples and it was found that the Fe(III)-activated SPC has a great potential in effective remediation of benzene-contaminated groundwater while more further studies should be done for its practical application in the future because of the complex subsurface environment.

15.
Purinergic Signal ; 12(3): 489-96, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27105971

RESUMO

P2X2 receptors, with other P2X receptor subtypes, have an important role mediating synaptic transmission in regulating the functions of the gastrointestinal tract. Our recent work has found a new regulator of P2X receptor function, called phosphoinositide-interacting regulator of transient receptor potential channels (Pirt). In the present work, we have shown that Pirt immunoreactivity was localized in nerve cell bodies and nerve fibers in the myenteric plexus of the stomach, ileum, proximal, and distal colon and in the submucosal plexus of the jejunum, ileum, proximal, and distal colon. Almost all the Pirt-immunoreactive (ir) neurons were also P2X2-ir, and co-immunoprecipitation experiments have shown that Pirt co-precipitated with the anti-P2X2 antibody. This work provides detailed information about the expression of Pirt in the gut and its co-localization with P2X2, indicating its potential role in influencing P2X2 receptor function.


Assuntos
Proteínas de Transporte/biossíntese , Sistema Nervoso Entérico/metabolismo , Proteínas de Membrana/biossíntese , Receptores Purinérgicos P2X2/biossíntese , Animais , Western Blotting , Imuno-Histoquímica , Imunoprecipitação , Masculino , Camundongos , Camundongos Endogâmicos C57BL , Camundongos Knockout
16.
Chem Eng J ; 302: 187-193, 2016 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-28943778

RESUMO

The ability of Fe(II)-activated calcium peroxide (CaO2) to remove benzene is examined with a series of batch experiments. The results showed that benzene concentrations were reduced by 20 to 100% within 30 min. The magnitude of removal was dependent on the CaO2/Fe(II)/Benzene molar ratio, with much greater destruction observed for ratios of 4/4/1 or greater. An empirical equation was developed to quantify the destruction rate dependence on reagent composition. The presence of oxidative hydroxyl radicals (HO•) and reductive radicals (primarily O2•-) was identified by probe compound testing and electron paramagnetic resonance (EPR) tests. The results of the EPR tests indicated that the application of CaO2/Fe(II) enabled the radical intensity to remain steady for a relatively long time. The effect of initial solution pH was also investigated, and CaO2/Fe(II) enabled benzene removal over a wide pH range of 3.0~9.0. The results of radical scavenging tests showed that benzene removal occurred primarily by HO• oxidation in the CaO2/Fe(II) system, although reductive radicals also contributed. The intermediates in benzene destruction were identified to be phenol and biphenyl. The results indicate that Fe(II)-activated CaO2 is a feasible approach for treatment of benzene in contaminated groundwater remediation.

17.
Chem Eng J ; 281: 286-294, 2015 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-26549979

RESUMO

The performance of Fe(III)-based catalyzed sodium percarbonate (SPC) for stimulating the oxidation of tetrachloroethene (PCE) for groundwater remediation applications was investigated. The chelating agents citric acid monohydrate (CIT), oxalic acid (OA), and Glutamic acid (Glu) significantly enhanced the degradation of PCE. Conversely, ethylenediaminetetraacetic acid (EDTA) had a negative impact on PCE degradation, which may due to its strong Fe chelation and HO• scavenging abilities. However, excessive SPC or chelating agent will retard PCE degradation. In addition, investigations using free radical probe compounds and radical scavengers revealed that PCE was primarily degraded by HO• radical oxidation in both the chelated and non-chelated systems, while O2•- also participated in the non-chelated system and the OA and Glu modified systems. According to the electron paramagnetic resonance (EPR) studies, the presence of HO• in the Fe(III)/SPC system was maintained much longer than that in the Fe(II)/SPC system. The results indicated that the addition of CIT, OA or Glu indeed enhanced the generation of HO• in the first 10 min and promoted degradation efficiency by increasing the amount of Fe(III) and maintaining the concentration of HO• radicals in solution. In conclusion, chelated Fe(III)-based catalyzed SPC oxidation is a promising method for the remediation of PCE-contaminated groundwater.

18.
Environ Technol ; 36(9-12): 1389-97, 2015.
Artigo em Inglês | MEDLINE | ID: mdl-25496173

RESUMO

Iron oxide-magnetite (Fe3O4) as a heterogeneous activator to activate persulphate anions (S2O8(2-)) for trichloroethylene (TCE) degradation was investigated in this study. The experimental results showed that TCE could be completely oxidized within 5 h by using 5 g L(-1) magnetite and 63 mM S2O8(2-), indicating the effectiveness of the process for TCE removal. Various factors of the process, including. (S2O8(2-) and magnetite dosages, and initial solution pH, were evaluated, and TCE degradation fitted well to the pseudo-first-order kinetic model. The calculated kinetic rate constant was increased with increasing S2O8(2-) and magnetite dosages, but it was independent of solution pH. In addition, the changes of magnetite morphology examined by scanning electron microscopy and X-ray powder diffraction, respectively, confirmed the slight corrosion with α-Fe2O3 coated on the magnetite surface. The probe compounds tests clearly identified the generation of the reactive oxygen species in the system. While the free radical quenching studies further demonstrated that •SO4- and •OH were the major radicals responsible for TCE degradation, whereas •O2- contributed less in the system, and therefore the roles of reactive oxygen species on TCE degradation mechanisms were proposed accordingly. To our best knowledge, this is the first time the performance and mechanism of magnetite-activated persulphate oxidation for TCE degradation are reported. The findings of this study provided a new insight into the heterogeneous catalysis mechanism and showed a great potential for the practical application of this technique in in situ TCE-contaminated groundwater remediation.


Assuntos
Óxido Ferroso-Férrico/química , Sulfatos/química , Tricloroetileno/química , Poluentes Químicos da Água/química , Oxirredução , Espécies Reativas de Oxigênio/química
19.
Environ Technol ; 35(5-8): 791-8, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-24645461

RESUMO

In this study, in-situ chemical oxidation technique employing Fe(II) catalytic sodium percarbonate (SPC) to stimulate the oxidation of trichloroethylene (TCE) in contaminated groundwater remediation was investigated. The effects of various factors including the SPC/TCE/Fe2+ molar ratio, the initial solution pH and the widely found constituents in groundwater matrix such as Cl(-), HCO3(-), SO4(2-) and NO3(-) anions and natural organic matters were evaluated. The experimental results showed that TCE could be completely oxidized in 5 min at 20 degrees C with a SPC/TCE/Fe2+ molar ratio of 5:1:10, indicating the significant effectiveness of the SPC/Fe2+ system for TCE removal. The initial solution pH value (from 3 to 11) has less influence on TCE oxidation rate. In contrast, Cl(-) and HCO3(-) anions had a negative effect on TCE removal in which HCO3(-) possesses a stronger influence than Cl(-), whereas the effects of both SO4(2-) and NO3(-) anions appeared to be negligible. With the 1.0-10 mg/L concentrations of humic acid in solution, slightly inhibitive effect was observed, suggesting that dissolved organic matters consumed less SPC and had a negligible effect on the oxidation of TCE in SPC/Fe2+ system. From the intermediate products' analyses and the released Cl(-) contents from TCE parent contaminant in solution, all the decomposed TCE had completely dechlorinated and led to carbon dioxide and hydrocarbon. In conclusion, Fe(II) catalytic SPC oxidation is a highly promising technique for TCE-contaminated groundwater remediation, but some complex constituents such as HCO3(-), in in-situ groundwater matrix should be carefully considered for its practical application.


Assuntos
Carbonatos/química , Compostos Ferrosos/química , Ferro/química , Tricloroetileno/química , Purificação da Água/métodos , Ânions/química , Dióxido de Carbono/química , Catálise , Cloro/química , Água Subterrânea , Substâncias Húmicas , Hidrocarbonetos/química , Concentração de Íons de Hidrogênio , Íons , Cinética , Oxigênio/química , Solventes/química , Temperatura , Fatores de Tempo , Poluentes Químicos da Água/química
20.
J Environ Sci (China) ; 26(5): 1188-94, 2014 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-25079650

RESUMO

Titanium dioxide (TiO2), which is the widely used photo-catalyst, has been synthesized by simple hydrothermal solution containing tetrabutyl titanate and hydrofluoric acid. The synthesized product has been applied to photo-degradation in aqueous phase of chlorinated solvents, namely tetrachloroethene (PCE), trichloroethene (TCE) and 1,1,1-trichloroethane (TCA). The photo-degradation results revealed that the degradation of these harmful chemicals was better in UV/synthesized TiO2 system compared to UV/commercial P25 system and UV only system. The photo-catalytic efficiency of the synthesized TiO2 was 1.4, 1.8 and 3.0 folds higher compared to the commercial P25 for TCA, TCE and PCE degradation, respectively. Moreover, using nitrobenzene (NB) as a probe of hydroxyl radical (·OH), the degradation rate was better over UV/synthesized TiO2, suggesting the high concentration of ·OH generated in UV/synthesized TiO2 system. In addition, ·OH concentration was confirmed by the strong peak displayed in EPR analysis over UV/synthesized TiO2 system. The characterization result using XRD and TEM showed that the synthesized TiO2 was in anatase form and consisted of well-defined sheet-shaped structures having a rectangular outline with a thickness of 4 nm, side length of 50 nm and width of 33 nm and a surface 90.3 m(2)/g. XPS analysis revealed that ≡Ti-F bond was formed on the surface of the synthesized TiO2. The above results on both photocatalytic activity and the surface analysis demonstrated the good applicability of the synthesized TiO2 nano-sheets for the remediation of chlorinated solvent contaminated groundwater.


Assuntos
Cloro/química , Nanoestruturas/química , Solventes/química , Titânio/química , Água/química , Microscopia Eletrônica de Transmissão , Fatores de Tempo , Poluentes Químicos da Água/química , Difração de Raios X
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