Electron beam irradiation (EBI) has been considered an advanced technology for the treatment of water and wastewater, whereas very few previous investigations reported its use for removing pharmaceutical pollutants. In this study, the degradation of fluoxetine (FLX), an antidepressant marketed as Prozac(®), was investigated by using EBI at FLX initial concentration of 19.4 ± 0.2 mg L(-1). More than 90 % FLX degradation was achieved at 0.5 kGy, with FLX below the detection limit (0.012 mg L(-1)) at doses higher than 2.5 kGy. The elucidation of organic byproducts performed using direct injection mass spectrometry, along with the results of ion chromatography, indicated hydroxylation of FLX molecules with release of fluoride and nitrate anions. Nevertheless, about 80 % of the total organic carbon concentration remained even for 7.5 kGy or higher doses. The decreases in acute toxicity achieved 86.8 and 9.6 % for Daphnia similis and Vibrio fischeri after EBI exposure at 5 kGy, respectively. These results suggest that EBI could be an alternative to eliminate FLX and to decrease residual toxicity from wastewater generated in pharmaceutical formulation facilities, although further investigation is needed for correlating the FLX degradation mechanism with the toxicity results.

Dissertação apresentada como parte dos requisitos para obtenção do Grau de Mestre em Ciências na Área de Tecnologia Nuclear -Aplicações Orientadora: Dra. Sueli Ivone Borrely SÃO PAULO 2014 Agradecimentos Agradeço primeiramente a Deus por todas as oportunidades que me concedeu até este momento da minha vida. À Drª Sueli pela orientação, ensinamentos e dedicação para a realização deste trabalho. E pela oportunidade da realização deste mestrado. Ao meu marido, Victor Hugo, pela paciência, compreensão e amor. Muito obrigada por sempre estar ao meu lado me apoiando e incentivando. Aos meus queridos pais, Sergio e Ivete, pelo enorme apoio e incentivo que a cada dia me motivam a seguir em frente. Sem vocês hoje eu nada seria. Aos meus irmãos, Camila e Rafael, que sempre estão por perto me ajudando. E que sempre poderão contar comigo para tudo. Aos meus avós: Akio (in memorian), Leico, Hiroyuki e Rosa. À minha segunda família: Cláudio, Joana, Marco e Sayuri. À Drª Ana Paula e ao Drº Antonio Carlos, da Engenharia Química (USP) pela grande ajuda nas análises químicas. Aos engenheiros responsáveis pelo acelerador de elétrons, Bete e Carlos, pelas irradiações das amostras. Ao técnico Reginaldo pela ajuda na manutenção do laboratório. Aos amigos do IPEN, Luana, Rejane, Aline, Daiane e Fernando. Ao IPEN pelo programa de pós-graduação. E ao CNPq pela bolsa de mestrado.Muito obrigada a todos! Toxicity and degradation assessment of the drug fluoxetine hydrochloride, in aqueous solution and mixed with domestic sewage, using electron beam irradiation AbstractExtensive use of drugs, lack of management in the production and disposal of these products as well as the difficulty in removing residues of pharmaceuticals during wastewater treatment phases imply the release of these micropollutants in water resources.Fluoxetine hydrochloride, known commercially as Prozac ® , have been often used in many countries. Studies demonstrate their presence in the environment and potential damage that this drug may cause the biota. Therefore, this paper studied a treatment technology (AOP -Advanced Oxidative Process) using ionizing radiation from an electron accelerator, for the degradation of the drug fluoxetine hydrochloride in aqueous solution and mixed with domestic sewage. After irradiation at aqueous solution chemical analyzes at the drug were done using spectrophotometry UV/VIS, Ultra Fast Liquid Chromatography (detectors UV/ VIS and fluorescence) and quantification of Total Organic Carbon (TOC). Acute toxicity tests (Daphnia similis and Vibrio fischeri) and chronic (Ceriodaphnia dubia) were employed. The efficiency for the degradation of the drug was greater than 98.00% at the lowest absorbed dose of radiation (0.5 kGy), however there was low rate of mineralization to the doses applied in this study. The efficiency reduction of toxicity was 83.75% using Daphnia similis at 0.5 kGy of absorbed dose and 87.24% at 5.0 kGy to fluoxetine hydrochloride, efficiency was 100.00% in reducing toxicity to domestic sewage and the mixture (CF + sewage) was...

No abstract

Photochemical advanced oxidation processes have been considered for the treatment of water and wastewater containing the herbicide atrazine (ATZ), a possible human carcinogen and endocrine disruptor. In this study, we investigated the effects of the photon emission rate and initial concentration on ATZ photolysis at 254 nm, an issue not usually detailed in literature. Moreover, the role of reactive oxygen species (ROS) is discussed. Photon emission rates in the range 0.87 × 10(18)-3.6 × 10(18) photons L(-1) s(-1) and [ATZ]0 = 5 and 20 mg L(-1) were used. The results showed more than 65 % of ATZ removal after 30 min. ATZ photolysis followed apparent first-order kinetics with k values and percent removals decreasing with increasing herbicide initial concentration. A fivefold linear increase in specific degradation rate constants with photon emission rate was observed. Also, regardless the presence of persistent degradation products, toxicity was efficiently removed after 60-min exposure to UV radiation. Experiments confirmed a noticeable contribution of singlet oxygen and radical species to atrazine degradation during photolysis. These results may help understand the behavior of atrazine in different UV-driven photochemical degradation treatment processes.