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1.
Water Res ; 44(7): 2245-52, 2010 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-20106498

RESUMO

This paper explores the degradation of a model pollutant, bisphenol A, by an advanced oxidation process that combines sonolysis, Fe(2+), and TiO(2) in a photoassisted process. Experiments were done under saturated oxygen conditions. The effect of different Fe(2+) (0.56 and 5.6 mg/L) and TiO(2) (10 and 50 mg/L) concentrations was investigated on both the elimination and mineralization of the pollutant. A pronounced synergistic effect that led to the complete and rapid elimination of dissolved organic carbon (DOC) was observed even at low catalyst loadings. In this system, almost a complete removal of DOC (93%) was observed after 4 h using 10 and 5.6 mg/L of TiO(2) and Fe(2+), respectively, whereas at the same time, only 5, 6, and 22% of DOC was removed by an individual process alone (TiO(2) photocatalysis, ultrasound, and photo-Fenton, respectively). In this system, ultrasound has the principal role of eliminating the initial substrate and providing hydrogen peroxide for the photocatalytic systems, while photo-Fenton and TiO(2) photocatalysis are mainly responsible for the transformation of the intermediates in CO(2) and H(2)O. The role of H(2)O(2) generated from the sonochemical process is also discussed.


Assuntos
Compostos Ferrosos/química , Fenóis/química , Titânio/química , Ultrassom , Poluentes Químicos da Água/química , Compostos Benzidrílicos , Catálise/efeitos da radiação , Peróxido de Hidrogênio/química , Ferro/química , Oxirredução/efeitos da radiação , Processos Fotoquímicos , Eliminação de Resíduos Líquidos/métodos
2.
Ultrason Sonochem ; 17(1): 111-5, 2010 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-19535280

RESUMO

Sonochemical elimination of organic pollutants can take place through two degradation pathways. Molecules with relatively large Henry's law constants will be incinerated inside the cavitation bubble, while nonvolatile molecules with low Henry's law constants will be oxidised by the OH(*) ejected from the bubble of cavitation. Taking bisphenol-A as a model pollutant, this study points out an alternate degradation route, mediated by bicarbonate ions, which is significant for the elimination of micro-pollutants at concentrations present in natural waters. In this process, OH(*) radicals react with bicarbonate ions to produce the carbonate radical, which, unlike the OH(*) radical, can migrate towards the bulk of the solution and therefore induce the degradation of the micro-pollutants present in the bulk solution. As a consequence, initial degradation rate is increased by a factor 3.2 at low concentration of bisphenol-A (0.022 micromol l(-1)) in presence of bicarbonate in water.


Assuntos
Poluentes Ocupacionais do Ar/química , Poluentes Ocupacionais do Ar/efeitos da radiação , Bicarbonatos/química , Bicarbonatos/efeitos da radiação , Fenóis/química , Fenóis/efeitos da radiação , Sonicação/métodos , Compostos Benzidrílicos , Simulação por Computador , Modelos Químicos , Doses de Radiação
3.
Ultrason Sonochem ; 15(4): 605-611, 2008 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-17822937

RESUMO

Bisphenol A (BPA), a chemical compound largely used in the plastics industry, can end up in aquatic systems, which it disturbs by its endocrine disrupting effect (EDE). This study investigated the BPA degradation upon ultrasonic action under different experimental conditions. The effect of saturating gas (oxygen, argon and air), BPA concentration (0.15-460 micromol L(-1)), ultrasonic frequency (300-800 kHz) and power (20-80 W) were evaluated. For a 118 micromol L(-1)-BPA solution, with the best performance obtained at 300 kHz, 80 W, with oxygen as saturating gas. In these conditions, BPA can be readily eliminated by the ultrasound process (approximately 90 min). However, even after long ultrasound irradiation times (9 h), more than 50% of chemical oxygen demand (COD) and 80% of total organic carbon (TOC) remained in the solution. Analyses of intermediates using HPLC-MS investigation identified several products: monohydroxylated bisphenol A, 4-isopropenylphenol, quinone of monohydroxylated bisphenol A, dihydroxylated bisphenol A, quinone of dihydroxylated bisphenol A, monohydroxylated-4-isopropenylphenol and 4-hydroxyacetophenone. The presence of these hydroxylated aromatic structures showed that the main ultrasonic BPA degradation pathway is related to the reaction of BPA with the *OH radical. After 2h, these early products were converted into biodegradable aliphatic acids.


Assuntos
Fenóis/química , Fenóis/efeitos da radiação , Compostos Benzidrílicos , Catálise , Cromatografia Líquida de Alta Pressão , Gases , Peróxido de Hidrogênio/química , Ferro , Cinética , Espectrometria de Massas , Fenóis/análise , Espectrometria de Massas por Ionização por Electrospray , Espectrofotometria Ultravioleta , Ultrassom
4.
Environ Sci Technol ; 41(1): 297-302, 2007 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-17265962

RESUMO

Bisphenol A (BPA), an organic compound largely used in the plastic industry as a monomer for production of epoxy resins and polycarbonate, is an emerging contaminant that is released in the environmentfrom bottles and packaging. BPA degradation (118 micromol L(-1)) under sonochemical conditions was investigated in this study, using a 300 kHz frequency, with a 80 W electrical power. Under these conditions, BPA was eliminated by the ultrasound process (-90 min). However, even after long ultrasound irradiation periods (10 h), more than 50% of chemical oxygen demand (COD) and 80% of total organic carbon (TOC) remained in the solution, indicating that most BPA intermediates are recalcitrant toward ultrasonic action. Accumulation of hydrogen peroxide from *OH and *OOH radical recombination was also observed. To increase the efficiency of BPA treatment, experiments combined ultrasound with Fe2+ (100 micromol L(-1)) and/or UV radiation (254 nm): Ultrasound/UV; Ultrasound/Fe2+; Ultrasound/UV/ Fe2+. Both UV and Fe2+ induced hydrogen peroxide dissociation, leading to additional *OH radicals and complete COD and TOC removal. Thus difficulties in obtaining mineralization of micropollutants like BPA through ultrasonic action alone, can be overcome by the Ultrasound/UV/ Fe2+ combination. Moreover, this technique was found to be the most cost-effective one. So, the integrated ultrasound-UV-iron(ll) process was shown to be of interest for the treatment of wastewaters contaminated with BPA.


Assuntos
Disruptores Endócrinos/química , Compostos Ferrosos/química , Fenóis/química , Ultrassom , Eliminação de Resíduos Líquidos/métodos , Poluição da Água/prevenção & controle , Compostos Benzidrílicos , Carbono/análise , Peróxido de Hidrogênio/análise
5.
Ultrason Sonochem ; 14(2): 117-21, 2007 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-16837230

RESUMO

Acoustic cavitation, induced by ultrasound, can be used to eliminate organic pollutants from water. This type of ultrasonic treatment of polluted water can be grouped with those generally referred to as advanced oxidative processes since it involves hydroxyl radicals. In this case these highly active species are generated from the dissociation of water and oxygen dissociation caused by cavitation bubble collapse. The cavitation induced degradation rates of organic compounds in water are mainly linked to their vapor pressure and solubility and here we will further explore these links by examining the degradation of a mixture of two materials with different physical properties, chlorobenzene and 4-chlorophenol. The results obtained when a dilute solution of a mixture of these compounds saturated with argon is subjected to sonication at 300 kHz, parallels previous observations achieved in an aerated aqueous medium at 500 kHz. The two compounds exhibit sequential degradation with the more volatile chlorobenzene entering the cavitation bubble and being destroyed first. The 4-chlorophenol degradation occurs subsequently only when the chlorobenzene has been completely destroyed. The two compounds exhibit different behavior when sonicated in water saturated with oxygen. Under these conditions the two compounds are degraded simultaneously, a remarkable result for which two explanations can be proposed, both of which are based on the formation of additional OH radical species: The ability to produce conditions for the simultaneous elimination of two organic compounds by the use of oxygen is of great importance in the developing field of ultrasonic water treatment.


Assuntos
Hidrocarbonetos Aromáticos/química , Hidrocarbonetos Aromáticos/efeitos da radiação , Modelos Químicos , Modelos Moleculares , Oxigênio/química , Oxigênio/efeitos da radiação , Sonicação , Simulação por Computador , Soluções , Volatilização , Água/química
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