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.
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.
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.
Toxicity removal of pharmaceuticals mixtures through electron beam irradiation
2021 - BOIANI, N.F.; TOMINAGA, F.K.; BORRELY, S.I.
Is ionizing radiation effective in removing pharmaceuticals from wastewater?
2021 - TOMINAGA, FLAVIO K.; SILVA, THALITA T.; BOIANI, NATHALIA F.; JESUS, JULIANA M.S. de; TEIXEIRA, ANTONIO C.S.C.; BORRELY, SUELI I.
Wastewater and effluent discharges are the main causes of receiving water body pollution and important challenges in water quality management. Among the emerging contaminants, pharmaceuticals have increasingly drawn attention due to their incomplete removal during conventional biological treatment, inducing potential and actual risks to living organisms following residue discharges in river effluent. Electron beam irradiation (EBI) is a clean process technology for organic compound degradation and mineralization, as well as persistent pollutant detoxification. This study aimed to evaluate EBI effects on the degradation and toxicity removal of anti-inflammatory aspirin (ASA) in a single solution and in a fluoxetine (FLX) mixture. Results indicate that 98% of the single aspirin was degraded at 5.0 kGy. Aspirin toxicity to Daphnia similis, however, increased with increasing absorbed dose (1.0 to 5.0 kGy), possibly as a result of the presence of H2O2 and other byproducts formed during the oxidation process. Regarding the irradiated mixture, complete degradation was achieved for both pharmaceuticals. Toxicity removals for the mixture were of 56.2 ± 0.9% and 58.8 ± 5.4% for 1.0 and 2.5 kGy, respectively. These findings demonstrate that EBI can be an interesting alternative process to be applied as a pre-treatment followed by biological treatment.
Evaluation of toxicity and color reduction of Reactive dye Yellow 160 and Red BG-3B, and textiles effluents after treatment by electron beam
2017 - GARCIA, V.; SOLE, S.V.; BOIANI, N.F.; ROSA, J.M.; BORRELY, S.I.
Textile effluents are always collored due to the amount of dyes lost during dieying processes. The low biodegradability and high solubility makes these compounds (reactive dyes) difficult to be enough removed by conventional treatment processes. The objective of the present study is to assess toxicity of Reactive dye Yellow - 160 and Red BG-3B as well as raw effluents containing such dyes. Acute toxicity tests were carried out with reference aquatic organisms: Vibrio fischeri bacteria and Daphnia similis microcrustaceans. After this, the effluent is also submitted to EBI treatment (irradiation at electron beam accelerator) for reducing color, with 0.5 kGy to 20 kGy doses. 100% of daphnids survived at 1g.L-1 of RY-160, and for Red BG-3B (C=0.564 g.L-1) EC 50% (48h) = 69.0 ± 0.66 . Raw textile effluent with dye RY-160 resulted in EC 50% lower than 2% for both organisms (D. similis EC 50% (48h) = 1.74 ± 0.53 and 0.6 ± 0.29, V. fischeri (15 min). For raw textile with Red BG-3B: D. similis EC 50% (48h) = 6.73 ± 0.72. The EBI treatment was effective for color removal, efficiency superior to 90% at 10 kGy. The data demonstrated the importance of evaluating not only dyes but also the effluent, since it has several additives that contributed to the high toxicity.
Toxicity assessment of caffeine, fluoxetine and their mixture on Daphnia similis
2019 - BOIANI, N.F.; SILVA, T.T.; BORRELY, S.I.
Emerging pollutants have already become a global problem, and they have been detected in dozens of countries, including Brazil. Even at very low concentrations, most of the emerging compounds are able to induce changes into biochemical system of aquatic organisms and they have also been reported as negative products to human health. Pharmaceuticals are considered as emerging contaminants detected in estuarine environment, in wastewater treatment facilities, lakes and rivers and even in sea waters. Generally the pharmaceuticals are detected among many other compounds into the ecosystem. The interaction of mixtures of contaminants is an important issue to be considered in monitoring programs as well as the negative effect to aquatic biota. The aim of the present paper was the assessment of toxic effects of pharmaceuticals exposed to Daphnia similis crustacean, individual and combined mixture of caffeine and fluoxetine. Caffeine (CAF) is a stimulant with cardiac, cerebral, diuretic and respiratory effects while Fluoxetine (FLX) is a selective serotonin re-uptake inhibitor, widely prescribed as antidepressant, (also known as Prozac®). The juveniles of D. similis were exposed separetaly to both caffeine (100mg/L) and to fluoxetine (20mg/L), and to a mixture of both (50mg/L caffeine and 20mg/L fluoxetine). Several experimental trials of acute immobilization test were performed. EC50 values ranged from 29,7 to 31 mg/L-1 for caffeine, and from 1.0 to 1.4 mg/L-1 for fluoxetine. Antagonistic effects of binary mixtures (EC50 = 15.2%) were observed. A chronic reproduction test was performed for the mixture of pharmaceuticals. We observed effects on D.similis survival, after 5 days. The mixture led to decrease of 72% in the reproduction, in maximum concentration (2.5% of the mixture – CAF 50ppm + FLX 20ppm). Concerning the importance of assessing toxicity the elected pharmaceuticals concentration were higher than those detected in the envinroment. These results may be incorporated into risk assessments analysis in order to protect sensitive aquatic ecosystems more effectively.