NATHALIA FONSECA BOIANI

NATHALIA FONSECA BOIANI

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Toxicity removal of pharmaceuticals, fluoxetine and caffeine, by electron beam irradiation
2023 - BOIANI, NATHALIA F.; REDIGOLO, MARCELO M.; CALVO, WILSON A.; TOMINAGA, FLAVIO K.; BORRELY, SUELI I.
The wide use of pharmaceuticals and water scarcity are associated to increasing levels of pharmaceutical compounds discharged into water and wastewater worldwide, affecting relevant ecological services, including biodegradation. However, water pollution has also encouraged studies applying advanced oxidative processes (AOP) in organic pollutant degradation. Among AOPs, ionizing radiation has been proven an effective technology for organic compound removal from waters and wastewater. The objective of this study was to assess Electron Beam (EB) irradiation in the degradation of caffeine and fluoxetine and their binary mixture in pure aqueous solutions. The degradation of these pharmaceuticals was evaluated by GC/MS analyses. The degradation dose response was higher for the caffeine and fluoxetine mixture (1:1) at 2.5 kGy. This dose led to decreased toxicity towards Daphnia similis for both the fluoxetine + caffeine mixture and the isolated fluoxetine solution, but not for the isolated caffeine. On the other hand, Vibrio fischeri exposure for 15 min indicated toxicity removal for the entire pharmaceuticals sample set and radiation dose. Fluoxetine was the most toxic pharmaceutical, followed by the binary mixture. Thus, we suggest ecopharmacovigilance, where attention should be paid to the increasing amount of pharmaceuticals, caffeine and fluoxetine detected in water.
Avaliação da toxicidade aguda e dos efeitos da irradiação com feixe de elétrons em misturas de compostos farmacêuticos
2022 - BOIANI, NATHALIA F.
Atualmente uma vasta gama de contaminantes vêm sendo detectados no meio hídrico, os produtos farmacêuticos merecem atenção especial, pois representam mistura complexa de contaminantes no ambiente, podendo causar efeitos deletérios a biota. Esses compostos possuem alta produção, utilização, descarte incorreto, chegando a rede coletora de esgoto através principalmente, da excreção humana e de residuos da indústria farmaceutica e agropecuária. Em águas superficiais, contribuem na alteração do padrão de qualidade das águas e redução da biodiversidade de organismos aquáticos, afetando tanto os ecossistemas quanto a saúde humana. As técnicas convencionais de tratamentos de efluentes são insuficientes na remoção desses compostos e seus metabólitos, sendo assim, buscam-se técnicas avançadas capazes de reduzir esses resíduos nas águas. O processo de irradiação por feixe de elétrons vem mostrando resultados satisfatórios na degradação dos compostos farmacêuticos, podendo ser utilizado como alternativa ou complemento aos processos de tratamento de efluentes. O objetivo deste trabalho foi a avaliação ecotoxicológica de quatro compostos farmaceuticos, isolados e em diferentes misturas (binárias, ternárias e quaternárias), bem como a aplicação da irradiação por feixe de elétrons, como proposta de tratamento para a redução dos efeitos tóxicos. Foram realizados ensaios com o antidepressivo Fluoxetina, o β-bloqueador Propranolol, o antibiótico Sulfadiazina e o estimulante Cafeína, individuais e combinados, antes e após o processo de irradiação. Os organismos-teste utilizados foram o microcrustáceo Daphnia similis e a bactéria Vibrio fischeri. A avaliação de risco através da concentração prevista sem efeito (PNEC), e a interação das misturas binárias (MixTox) também foram abordados no presente estudo. Os resultados dos ensaios de toxicidade para efeitos agudos dos fármacos individuais indicaram possível risco de sua presença para a biota aquática, quanto ao Propranolol e a Cafeína. Nas análises das interações toxicológicas das misturas binárias, foi identificado sinergismo para a mistura de Fluoxetina com Propranolol, e antagonismo para a mistura de Fluoxetina com Sulfadiazina e com a Cafeína. A irradiação por feixe de elétrons foi eficaz na redução da toxicidade dos compostos combinados. Na mistura binária de Fluoxetina com o Propranolol, a eficiência de remoção da toxicidade foi de 80% para D. similis e 30% para V. fischeri, nas doses de 2,5 e 5,0 kGy. A mistura de Fluoxetina com Sulfadiazina apresentou valores entre 20-30% de redução da toxicidade para ambos os organismos e doses aplicadas. Os resultados da mistura de Fluoxetina com Cafeína apresentaram eficiência de remoção da toxicidade de 45% para D.similis e 30% para V.fischeri, nas doses aplicadas. Nas misturas ternárias, a eficiência de remoção de toxicidade foi de 40% e 55% para V. fischeri, e de 25% e 35% para D. similis, respectivamente nas doses de 2,5 e 5,0 kGy. Na mistura quaternária a redução da toxicidade chegou a 80% para V. fischeri versus 60% para D. similis, na dose de 5,0 kGy; e em 40%, para ambos os organismos, na dose de 2,5 kGy. Houve o decaimento da absorbância em todos os comprimentos de onda característicos das amostras, indicando que o processo de irradiação foi eficiente na degradação dos compostos, porém baixa eficiência de remoção de carbono orgânico total, indicando que não houve mineralização significativa das amostras irradiadas.
Electron beam irradiation applied for the detoxification and degradation of single ciprofloxacin aqueous solution and multiclass pharmaceutical quaternary mixture
2023 - TOMINAGA, FLAVIO K.; BOIANI, NATHALIA F.; SILVA, THALITA T.; SANTOS, JONAS G. dos; LEBRE, DANIEL T.; LEO, PATRICIA; BORRELY, SUELI I.
The application of electron beam irradiation for detoxification and degradation of single antibiotic ciprofloxacin (CPF) and in a mixture with multiclass pharmaceuticals in aqueous solutions was carried out. Ecotoxicity assays indicated that the green algae were most sensitive to antibiotic and also that the presence of several pharmaceutical increased the toxicity. After the irradiation treatment, degradation results of single antibiotic indicated reduction of 95.86 % at 1.0 kGy. Total organic carbon decreased up to 38 % at 5.0 kGy. At lower doses (1.0 kGy), no effect in toxicity was evidenced, however, increase in toxicity for Vibrio fischeri was observed after 2.5 kGy. For Daphnia similis exposure, an increase in toxicity was noted for all applied doses. In contrast, for the green algae R. subcapitata toxicity reduction varied from 62.3 to 81.9 % at the evaluated doses. Toxicity assays to microbes E. coli and S. aureus reduced antibacterial activity of CPF after irradiation treatment. Regarding the irradiated quaternary mixture at 2.5 kGy, reduction up to 96 % was achieved for the ciprofloxacin, metformin and acetylsalicylic acid, and 81 % removal was achieved for fluoxetine. Acute assays with V. fischeri indicated no increase in toxicity, while some increase was noted for D. similis (acute effects). Nevertheless, chronic assays data indicated low toxicity reduction (14 %) with D. similis, and complete detoxification was shown for the green algae after the irradiation. In addition, decrease in antimicrobial activity was noted after the treatment. Furthermore, the in-silico model was not enough accurate for the prediction of CIP toxicity. These findings showed that electron beam irradiation can be applied for reducing the impacts of antibiotics in aquatic ecosystem. Measuring toxicity on living-organism from different trophic levels are useful tools to evaluate the interaction of mixtures and also to assess toxicity of the generated byproducts.
Application of electron beam irradiation for remediation of pharmaceutical compounds in water
2022 - TOMINAGA, F.K.; BOIANI, N.F.; SILVA, T.T.; LEO, P.; BORRELY, S.I.
A significant number of pharmaceutical active compounds have been released in the aquatic environment. These compounds are not fully removed from water and wastewater treatment plants. Furthermore, these contaminants are not commonly monitored, and they possess the potential to cause adverse ecological and human health effects. Electron Beam Irradiation (EBI) have been applied as an alternatively green method in water management, being efficient for removing organic recalcitrant pollutants at low doses. This work aims to assess the effect of EBI on toxicity of four pharmaceuticals from distinct class (anti-inflammatory, antidepressant, antibiotic, and antidiabetic) using organism from different trophic levels. Acetylsalicylic acid and fluoxetine hydrochloride were obtained from Labsynth (>99.5%) and Divis Pharmaceuticals Pvt. Ltd (98.8%), respectively. Metformin hydrochloride (97%) and ciprofloxacin (>98%) were purchased from Sigma- Aldrich. All aqueous solution were diluted using ultra-pure water. Acute toxicity assays with Daphnia similis and Vibrio fischeri were based on ABNT/NBR standard methods. The evaluated endpoint was immobility and bioluminescence inhibition, respectively. The yeast assays were carried by monitoring of changes in the specific conductivity of suspensions of S. cerevisiae. All the assays were performed in triplicate. The toxicity results of the microcrustacean and the bacteria were expressed in Toxicity Factor. For the yeast, data were analyzed by F-test and t-test using a significance level of 0.05. The UV-Vis spectrum showed changes in all pharmaceutical’s spectrum after irradiation at 2.5 kGy. The toxicity results indicated that the effects varied depending on the organism and the studied pharmaceutical. For acetylsalicylic acid, increase of toxicity was observed for all three the organism. In contrast, for fluoxetine, a great toxicity removal was achieved for D. similis while and for the bacteria and the yeast no changes of toxicity were noted. Regarding metformin, the radiolytic byproducts were only toxic to the microcrustacean, possibly including residual hydrogen peroxide. Finally, for ciprofloxacin, toxicity increase was verified for D. similis and V. fischeri, while detoxification was observed for S. cerevisiae. In conclusion, the present work demonstrated EBI is effective for removing pharmaceuticals and showed the importance of using different organism for toxicity assessment.
Assessment of binary mixture toxicity of pharmaceuticals of environmental concern to aquatic organisms
2022 - BOIANI, N.F.; TOMINAGA, F.K.; SILVA, T.T.; REDÍGOLO, M.M.; BORRELY, S.I.
Pharmaceutical products have been frequently detected in aquatic environments as mixtures. They may cause direct toxic effects to aquatic organisms and indirect effects on ecosystems, due to interactions which induce additive, synergistic or antagonistic effects. The classical mathematical models of concentration addition and independent action of pollutants have been extensively used for predicting the mixture effects of chemicals of environmental relevance. The objective of this study was to assess the binary mixture toxicity of pharmaceuticals: fluoxetine and propranolol; fluoxetine and sulfadiazine; fluoxetine and caffeine, in acute tests with Daphnia similis carried out based on ABNT/NBR standard methods. The prediction of the acute effects to binary mixture was performed considering the mentioned mathematical models and deviations of them (synergism/antagonism; concentration level-dependent or concentration ratio-dependent), using an automated Excel spreadsheet. For the mixture of propranolol + fluoxetine, the concentration addition model best described the mixture effects, which explained most of the variability of acute toxic responses. Through the concentration level-dependent, synergism at low doses and antagonism at high doses was pointed out. The concentration addition model better described the effects of the binary mixture of sulfadiazine + fluoxetine. Synergism related to the independent action model and an antagonism related to the concentration ratio-depend were identified. For caffeine + fluoxetine mixture, the concentration addition model described slightly better the effects of this binary mixture, synergism concentration level-dependent and dose ratio-dependent were identified. We can conclude that the nature of the interaction between the compounds of a mixture depends on effect level and on the ratio in which each one is applied. Major effects of the binary mixture were detected in the zone between the effects predicted by the evaluated models. The synergism/antagonism or additivity do not depend on the similarity/dissimilarity of the mode of action of the compounds of a mixture, showing a different behaviour respect to the theoretical assumptions.
Toxicidade aguda e avaliação de riscos ecológicos de fármacos pertencentes a diferentes classes detectados em ambientes aquáticos
2021 - TOMINAGA, F.K.; BOIANI, N.F.; GARCIA, V.S.G.; SILVA, T.T.; LEO, P.; BORRELY, S.I.
Avaliação da toxicidade da mistura de fármacos submetidos a irradiação por feixe de elétrons
2021 - BOIANI, N.F.; SILVA, T.T.; TOMINAGA, F.K.; GARCIA, V.S.G.; BORRELY, S.I.
Toxicity removal of pharmaceuticals mixtures through electron beam irradiation
2022 - BOIANI, N.F.; TOMINAGA, F.K.; BORRELY, S.I.
Contamination of the aquatic environment by pharmaceuticals is becoming a global phenomenon of growing concern. Pharmaceuticals are partially metabolized, resulting in the excretion and release of residual into sewage, unaltered or metabolites. The wastewater treatment plants are not designed to eliminate these compounds, leading the residues into the aquatic environment. Besides, pharmaceuticals are not detected individually but as a complex mixture. Advanced oxidative processes have been applied as an alternative or complement to conventional sewage treatment processes, aiming the degradation and removal of toxic pollutants. The objective of this study was to evaluate the toxicity removal of mixtures of pharmaceuticals subjected to electron beam treatment. The aqueous solutions of each pharmaceutical were diluted in ultra-pure water and prepared in three pharmaceuticals combinations: Propranolol + Fluoxetine + Sulfadiazine; Propranolol + Fluoxetine + Diclofenac; Acetylsalicylic acid + Fluoxetine + Metformin). Electron Beam Accelerator was applied for the irradiations and the absorbed doses were 2.5-5.0 kGy. Acute toxicity tests with Daphnia similis were performed to evaluate the toxicity, before and after irradiation.. The data analyzed showed toxicity removal efficiency around 80% for the mixture of Propranolol, Fluoxetine and Diclofenac; 75% for the mixture of Propranolol, Fluoxetine and Sulfadiazine; and 30% for the mixture of Acetylsalicylic acid, Fluoxetine and Metformin. According to the literature, this is a viable technology for the removal of toxicity from pharmaceuticals, and the results demonstrated the potential of electron beam irradiation in reducing the toxicity of pharmaceutical from different classes.
Acute and chronic ecotoxicological effects of pharmaceuticals and their mixtures in Daphnia similis
2022 - TOMINAGA, FLAVIO K.; BOIANI, NATHALIA F.; SILVA, THALITA T.; GARCIA, VANESSA S.G.; BORRELY, SUELI I.
Pharmaceuticals have increasingly received attention from the scientific community due to their growing intake, improved detection and potential ecological risks. Several pharmaceuticals, including antidepressants, anti-inflammatory and antidiabetic compounds and antibiotics, have been described as contaminants in different water matrices. In this context, the aim of the present study was to assess the acute and chronic effects of four classes of pharmaceuticals (acetylsalicylic acid, fluoxetine, metformin and ciprofloxacin) individually and in binary and quartenary mixture. Furthermore, the toxicity of binary mixtures containing the antidepressant fluoxetine was also evaluated. The results of the single acute and chronic toxicity assays indicate lower acetylsalicylic acid and higher fluoxetine toxicity towards Daphnia similis. Regarding the evaluated mixture toxicity, the nature of potential toxicological interactions was predicted by applying mathematical concentration addition and independent action models. The findings revealed both antagonistic and synergistic features, depending on the applied amounts and doses. Finally, the chronic assays performed with the quaternary mixture indicated the presence of a hormetic effect at low concentrations. In sum, the present study demonstrated that the effects of individual pharmaceuticals can underestimate the risk level of these contaminants in the environment.
Gas chromatography-mass spectrometry analysis of irradiated fluoxetine aqueous samples
2021 - REDÍGOLO, MARCELO M.; CALVO, WILSON A.P.; BOIANI, NATHALIA F.; TOMINAGA, FLAVIO K.; BORRELY, SUELI I.
The last decade witnessed the drastic increase in the use of antidepressant drugs, being fluoxetine the most prescribed worldwide. Conventional wastewater treatment is inefficient in removing fluoxetine and its accumulation in water bodies and water living organism is inevitable. Among several methods for contaminant removal from wastewater, electron beam irradiation is an efficient and green technology. This work presents the characterization of aqueous fluoxetine samples before and after irradiation. Gas chromatography coupled to mass spectrometry was used to identify the original compound and its irradiation products. Results indicate a drastic reduction in fluoxetine presence after the irradiation process. Radiolysis pathways were proposed based on mass fragments identification.