FLAVIO KIYOSHI TOMINAGA

FLAVIO KIYOSHI TOMINAGA

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BDD-persulfate-based anodic oxidation process for progestin degradation
2024 - JESUS, JULIANA M.S. de; ARGOLO, ALLAN dos S.; TOMINAGA, FLAVIO K.; BILA, DANIELE M.; BORRELY, SUELI I.; TEIXEIRA, ANTONIO C.S.C.
Considering the increasing presence of the hormones levonorgestrel (LNG) and gestodene (GES) in wastewater, the limited effectiveness of conventional treatment methods, and the demand for advanced complementary processes, our study aimed to optimize an anodic oxidation treatment with a focus on low specific energy consumption (SEC) and costs. An electrochemical system coupled to a boron-doped diamond anode (BDD) was continuously used to treat synthetic and real pharmaceutical wastewater from contraceptive production. The central design composite and response surface methodology were the tools employed for optimization. The lowest SEC was obtained as a response to the main process variables: current density, initial pH, and the concentration of the support electrolyte ([Na2S2O8]). The optimal condition ([Na2S2O8]0 = 0.07 mol L−1; [LNG]0,RPW = 1.02±0.05 mg L−1 and [GES]0,RPW = 1.05±0.05 mg L−1; j = 37.5 mA cm−2; pH = 6.75) was established considering an SEC ≤ 3.6 ± 0.8 kWh g−1 and progestins removal ≥70%, which was the experimental condition used to evaluate acute toxicity to Daphnia similis and the effect on estrogenic activity removal using the YES assay. Notably, our study evaluated, for the first time, a comparative investigation that highlights the substantial effect of support electrolytes over the eco-compatibility assessment of the anodic oxidation process investigated. The adaptability of the operation indicates the prospective suitability for the implementation of the process in wastewater treatment facilities in the pharmaceutical industry.
Emerging pollutants in textile wastewater
2024 - GARCIA, VANESSA S.G.; TOMINAGA, FLAVIO K.; ROSA, JORGE M.; BORRELY, SUELI I.
Water and several chemicals, including dyestuffs, surfactants, acids, and salts, are required during textile dyeing processes. Surfactants are harmful to the aquatic environment and induce several negative biological effects in exposed biota. In this context, the present study aimed to assess acute effects of five surfactants, comprising anionic and nonionic classes, and other auxiliary products used in fiber dyeing processes to aquatic organisms Vibrio fischeri (bacteria) and Daphnia similis (cladocerans). The toxicities of binary surfactant mixtures containing the anionic surfactant dodecylbenzene sulfonate + nonionic fatty alcohol ethoxylate and dodecylbenzene sulfonate + nonionic alkylene oxide were also evaluated. Nonionic surfactants were more toxic than anionic compounds for both organisms. Acute nonionic toxicity ranged from 1.3 mg/L (fatty alcohol ethoxylate surfactant) to 2.6 mg/L (ethoxylate surfactant) for V. fischeri and from 1.9 mg/L (alkylene oxide surfactant) to 12.5 mg/L (alkyl aryl ethoxylated and aromatic sulfonate surfactant) for D. similis, while the anionic dodecylbenzene sulfonate EC50s were determined as 66.2 mg/L and 19.7 mg/L, respectively. Both mixtures were very toxic for the exposed organisms: the EC50 average in the anionic + fatty alcohol ethoxylate mixture was of 1.0 mg/L ± 0.11 for V. fischeri and 4.09 mg/L ± 0.69 for D. similis. While the anionic + alkylene oxide mixture, EC50 of 3.34 mg/L for D. similis and 3.60 mg/L for V. fischeri. These toxicity data suggested that the concentration addition was the best model to explain the action that is more likely to occur for mixture for the dodecylbenzene sulfonate and alkylene oxide mixtures in both organisms. Our findings also suggest that textile wastewater surfactants may interact and produce different responses in aquatic organisms, such as synergism and antagonism. Ecotoxicological assays provide relevant information concerning hazardous pollutants, which may then be adequately treated and suitably managed to reduce toxic loads, associated to suitable management plans.
Toxicological response of Saccharomyces cerevisiae to acetylsalicylic acid aqueous solution treated by electron beam irradiation
2023 - TOMINAGA, FLAVIO K.; LEO, PATRICIA; BORRELY, SUELI I.
Pharmaceuticals have drawn attention due to the potential of causing negative impacts on the population and ecosystems at ecological relevant concentrations. Among these contaminants, acetylsalicylic acid is a drug widely used in human medicine as an analgesic, antipyretic and in actively preventing blood platelet aggregation, which has been introduced into the environment continuously. Several technologies have been proposed for the removal of contaminants. Electron beam irradiation (EBI) has been applied as an alternative and clean technology for pollutant removal. Nevertheless, after any type of treatment there may occur the formation of more toxic byproducts, which may be detected by biological assays. The Saccharomyces cerevisiae yeast consists in simple eukaryotic model, widely used for the assessment of toxic effects on human cells and tissues. This work aims the toxicity assessment of treated acetylsalicylic aqueous solutions by EBI employing Saccharomyces cerevisiae. Toxicity assays were performed with S. cerevisiae and the results were compared to others aquatic organisms (Vibrio fischeri bioluminescent bacteria and Daphnia similis microcrustacean). The results showed low sensibility to the yeast when exposed to the anti-inflammatory, demonstrating an EC5030min of 815 mg L-1, when compared with the bioluminescent bacteria (EC5015min = 38.48 mg L-1) and the microcrustacean (EC5048h = 86.05 mg L-1). Due to low acute toxicity, chronic assays were also performed with D. similis, demonstrating a NOEC14days of 2.5 mg L-1. Based on these results, toxicity data from chronic assays was utilized for PNEC estimation, and the highest concentration detected in Brazilian surface water was used to evaluate the worst-case scenario. The calculated risk quotient indicated a possible risk of acetylsalicylic acid to aquatic biota. After EBI treatment, increase in toxicity have been noted for all the evaluated organisms, indicating sensibility of the evaluated organism. This work demonstrated the feasibility of employing toxicity assays with the Saccharomyces cerevisiae yeast.
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.
Experimental design and bioassays as tools to investigate the impact of anodic oxidation on progestins degradation
2023 - JESUS, JULIANA M.S. de; ARGOLO, ALLAN dos S.; TOMINAGA, FLAVIO K.; TAQUEDA, MARIA E.; BILA, DANIELE M.; BORRELY, SUELI I.; TEIXEIRA, ANTONIO C.S.C.
The present study investigated the degradation of levonorgestrel (LNG) and gestodene (GES) through an anodic oxidation process mediated by active chlorine species. The independent variables [LNG]0 and [GES]0, current density (mA cm−2), and [NaCl]0 (mol L−1) were optimized through a response surface methodology (RSM) based on a four-level central composite design (CCD). Specific energy consumption allowed CCD-RSM analysis and optimization. The decay of progestins was followed to verify the kinetics of the anodic degradation process. Chlorine monitoring showed that excess Cl− concentration did not mean high hormones removal, as well as the excess of current density. Central point conditions ([NaCl]0 = 0.07 mol L−1, j = 32.5 mA cm−2, [LNG]0, and [GES]0 1.0 mg L−1) proved to be the best operational option. The performance with real pharmaceutical wastewater confirmed model optimization (2.2 ± 0.2 kWh g−1, with removals of 83.1 ± 0.9% and 75.1 ± 2.8% for LNG and GES, respectively). The selected condition was used for estrogenic activity and acute toxicity assays. The first allowed the identification of the initial estrogenic activity for the mixture of LNG and GES (924 E2-EQ ng L−1). Additionally, the electrochemical process could decrease this environmental parameter by 74.6%. The progestin mixture was classified as acute toxicity to Daphnia similis, with a toxicity unit (TU) of 2.5 100/EC50%. After electrolysis, the hormone solutions reached a fourfold increase in TU value, classified as high acute toxicity.
Investigation of persulfate-based AOPs to decontaminate water with a mixture of fluoxetine and levonorgestrel
2022 - SOUZA, L.P.; JESUS, J.M.S.; TOMINAGA, F.K.; RAMOS, B.; BORRELY, S.I.; TEIXEIRA, A.C.S.C.
This work reports a study on two forms of persulfate activation (solar irradiation and anodic oxidation-AO) for the degradation of active pharmaceutical ingredients (APIs). A solution containing a mixture of levonorgestrel and fluoxetine ([LNG]0 = 0.29 ± 0.03 mg L-1; [FLX]0 = 5.02 ± 0.34 mg L-1) was treated with persulfate ([PS]0 = 0.07 mol L-1) and irradiated or electrolyzed for 60 min under similar conditions. The results revealed similar decays of APIs in the two activation forms studied, solar/PS (k LNG = 6.6 × 10-2 min-1; k FLX = 7.7 × 10-2 min-1) and AO/PS (k LNG = 7.8 × 10-2 min-1; k FLX = 9.7 × 10-2 min-1), with slightly better results for the electrochemical process. However, acute toxicity accessed with Daphnia similis indicated that AO/PS provided a three-fold increase in the values of toxic units.
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.
Degradation and toxicity of amoxicillin after electron beam irradiation
2022 - BORRELY, S.I.; REDÍGOLO, M.M.; VILLARD, B.D.; LEBRE, D.T.; TOMINAGA, F.K.
A recent and growing concern in environmental studies is the presence of antibiotics in wastewater, which contributes to antimicrobial resistance building. Amoxicillin, according to the World Health Organization, is one of the most consumed antibiotics worldwide, for being a first line therapy for common infections. Among several drug degradation methodologies, electron beam irradiation (EBI) is presented as an efficient and green treatment. This work presents data on amoxicillin degradation via EBI. Degradation rate was evaluated by LC/MS-MS, carbon removal efficiency was evaluated by TOC and ecotoxicity assays were performed employing Vibrio fischeri. Chromatographic results indicate an efficiency removal of 97.65% at 0.75 kGy and concentration below the limit of detection with increasing absorbed dose. Low mineralization (up to 10%) was achieved at 3.0 kGy. Regarding toxicity, approximately 81% of toxicity removal was obtained at 0.75 kGy and a decrease in efficiency was achieved with higher doses. In conclusion, results indicate the low doses (0.75 kGy) as most effective for drug removal employing EBI.
Radiolytic degradation of levonorgestrel and gestodene
2022 - JESUS, JULIANA M.S. de; TOMINAGA, FLAVIO K.; ARGOLO, ALLAN dos S.; NASCIMENTO, ANA C.G.; BORRELY, SUELI I.; VIEIRA, DANIEL P.; BILA, DANIELE M.; TEIXEIRA, ANTONIO C.S.C.
This study reports the feasibility of ionizing sources (60Co source and electron beam radiation) to degrade the progestins hormones levonorgestrel (LNG) and gestodene (GES) in synthetic solutions and real pharmaceutical wastewater (RPW). Doses of 0.5–100 kGy and dose rates of 2.5 and 10 kGy h−1 were applied. LNG was shown to be more recalcitrant than GES, with 90% removals achieved at doses around 7.7 kGy (LNG) and 1.6 kGy (GES) in model systems, with LNG showing greater reactivity with reducing species in γ-radiolyis, unlike GES. Furthermore, LNG removal remained around 60% in RPW at low doses, while more than 60% GES removal was observed for all doses. LNG and GES toxicities to Daphnia similis were absorbed dose-dependent, with low doses resulting in toxicity reductions of around 32% (LNG) and 42% (GES); in turn, high doses promoted a fourfold increase in toxicity. γ-radiolysis reduced the cytotoxic character of LNG to NIH-3T3-L1 cells, while non-irradiated or irradiated GES solutions did not exhibit any cytotoxic effect. Finally, the estrogenic activity, evaluated by the YES assay, was dose-dependent for both progestins, which may be related to the evolution of transformation products formed by water radiolysis in each case, decreasing for high doses.
Toxicity removal of pharmaceuticals mixtures through electron beam irradiation
2021 - BOIANI, N.F.; TOMINAGA, F.K.; BORRELY, S.I.