Uso de resíduo de mineração de ferro em processo foto-fenton heterogêneo para a degradação de sulfonamidas
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Data
2016-12-14
Autores
Ayala Durán, Saidy Cristina [UNESP]
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Universidade Estadual Paulista (Unesp)
Resumo
Este trabalho tem como objetivo avaliar a atividade catalítica de um rejeito de mineração de ferro para a degradação de micropoluentes presentes no meio aquático em processo foto-Fenton heterogêneo. Como poluentes alvos, foram estudados os fármacos: sulfatiazol (STZ) e sulfametazina (SMZ), fármacos de uso estendido no tratamento humano e veterinário. Esses fármacos têm sido detectados em concentrações de ng L-1 a μg L-1 em águas superficiais, subterrâneas, águas de abastecimento, além de Estações de Tratamento de Esgoto (ETE) onde por processos convencionais não conseguem ser eliminados devido à baixa biodegradabilidade ambiental. Foi realizado um planejamento fatorial 24 para determinar os efeitos dos parâmetros reacionais ̶ pH, concentração de peróxido de hidrogênio, dose de rejeito e tamanho de partícula ̶ sendo a variável resposta a porcentagem de degradação do fármaco quantificado por Cromatografia Liquida de Alta Eficiência (HPLC-DAD) com Limites de Detecção (LD) e de Quantificação (LQ) de 6 μg L-1 e 20 μg L-1, respectivamente. O rejeito de minério foi caracterizado por Difração de Raios- X (DRX), Microscopia Eletrônica de Varredura de Alta Resolução (MEV-FEG), Espectroscopia de fotoelétrons excitados por raios- X (XPS) e Área Superficial Específica (BET). O rejeito foi caracterizado separando-se em duas faixas de tamanho de partícula <180 e ≥180 μm, além do rejeito bruto (sem separar). O resíduo apresentou entre seus principais minerais Fe2O3, SiO2, P2O5, CeO2, TiO2, ZnO, MgO além de outros traços, sendo que não apresenta diferenças significativas na composição nas duas faixas. A condição ótima para a degradação foi em pH 2,5 com 1 mmol L-1 de peróxido de hidrogênio, dose de rejeito de 0,3 g L-1 e usando-se o rejeito bruto como catalisador. Os experimentos de degradação tanto no escuro, quanto irradiado, mostraram boas porcentagens de degradação para os dois fármacos estudados, com porcentagens acima do 50% no escuro e acima de 80% sob irradiação, com cinéticas de pseudo primeira ordem seguindo o modelo cinético de Langmuir- Hinshelwood (L-H) com (r = 0,9861 a 0,9964) com constantes Kaparente de 0,0869 ± 0,0084 e 0,0718 ± 0,0035 para o STZ e SMZ respectivamente. Foi possível também a degradação simultânea de ambos os fármacos nas melhores condições experimentais. Considerando-se que não foi observada remoção por adsorção nem fotólise direita dos fármacos é possível afirmar que o rejeito de minério de ferro atua como catalisador eficiente em processos Fenton uma vez que altas porcentagens de degradação foram obtidas e pode ser um material promissor para esta aplicação, possibilitando agregar valor ao resíduo e diminuir o custo operacional do processo de tratamento.
This work aims to evaluate the catalytic activity of a residue from iron mining on the degradation of micropolluants present in the aquatic environment, by using the heterogeneous photo-Fenton process. The target pollutants studied was: sulfathiazole (STZ) and sulfamethazine (SMZ), drugs that are used in human and animal treatments, which has been detected in concentrations of ng.L-1 and ug.L-1 in superficial and underground water, human water supply and sewage treatment station where by conventional processes can’t be eliminated due to the low environmental biodegradability. A factorial design was performed 24 to determine the effects of the reaction parameters (pH, hydrogen peroxide concentration, residue dose and particle size). The response variable was the percentage of degradation of the drug, quantified by High Performance Liquid Chromatography (HPLC- DAD) with Detection Limits (DL) and Quantification (QL) of 6 μg L-1 and 20 μg L-1, respectively. Iron mining was characterized by X-ray diffraction (XRD), high resolution scanning electron microscopy (SEM), X-ray photoelectron Spectroscopy (XPS) and surface-specific spectroscopy (BET) spectroscopy. The reject was characterized by separating into two particles size < 180 and ≥ 180 μm in addition to the crude (unseparated) reject. The residue presented among its main minerals Fe2O3, SiO2, P2O5, CeO2, TiO2, ZnO, MgO in addition to other traces, and it does not present significant differences in the composition in the two different particle fractions. The optimum degradation condition was at pH 2.5 with 1 mmol L-1 of hydrogen peroxide, waste dose of 0.3 g L-1 and using the crude waste as catalyst. Both the dark and irradiated degradation experiments showed good percentages of degradation for the two drugs studied, with percentages above 50% in the dark and above 80% under irradiation, with pseudo first order kinetics following the Langmuir-Hinshelwood (L-H) kinetic model with (r = 0.9861 to 0.9964) with Kapp constants of 0.0869 ± 0.0084 and 0.0718 ± 0.0035 for STZ and SMZ respectively. It was also possible the simultaneous degradation of both drugs under the best experimental conditions. Considering that adsorption removal and direct photolysis of the drugs were not observed, it is possible to state that the iron ore acts as an efficient catalyst in Fenton processes since high percentages of degradation have been obtained, it can be a promising material for this application. Making it possible to add value to the waste and reduce the operational cost of the treatment process.
This work aims to evaluate the catalytic activity of a residue from iron mining on the degradation of micropolluants present in the aquatic environment, by using the heterogeneous photo-Fenton process. The target pollutants studied was: sulfathiazole (STZ) and sulfamethazine (SMZ), drugs that are used in human and animal treatments, which has been detected in concentrations of ng.L-1 and ug.L-1 in superficial and underground water, human water supply and sewage treatment station where by conventional processes can’t be eliminated due to the low environmental biodegradability. A factorial design was performed 24 to determine the effects of the reaction parameters (pH, hydrogen peroxide concentration, residue dose and particle size). The response variable was the percentage of degradation of the drug, quantified by High Performance Liquid Chromatography (HPLC- DAD) with Detection Limits (DL) and Quantification (QL) of 6 μg L-1 and 20 μg L-1, respectively. Iron mining was characterized by X-ray diffraction (XRD), high resolution scanning electron microscopy (SEM), X-ray photoelectron Spectroscopy (XPS) and surface-specific spectroscopy (BET) spectroscopy. The reject was characterized by separating into two particles size < 180 and ≥ 180 μm in addition to the crude (unseparated) reject. The residue presented among its main minerals Fe2O3, SiO2, P2O5, CeO2, TiO2, ZnO, MgO in addition to other traces, and it does not present significant differences in the composition in the two different particle fractions. The optimum degradation condition was at pH 2.5 with 1 mmol L-1 of hydrogen peroxide, waste dose of 0.3 g L-1 and using the crude waste as catalyst. Both the dark and irradiated degradation experiments showed good percentages of degradation for the two drugs studied, with percentages above 50% in the dark and above 80% under irradiation, with pseudo first order kinetics following the Langmuir-Hinshelwood (L-H) kinetic model with (r = 0.9861 to 0.9964) with Kapp constants of 0.0869 ± 0.0084 and 0.0718 ± 0.0035 for STZ and SMZ respectively. It was also possible the simultaneous degradation of both drugs under the best experimental conditions. Considering that adsorption removal and direct photolysis of the drugs were not observed, it is possible to state that the iron ore acts as an efficient catalyst in Fenton processes since high percentages of degradation have been obtained, it can be a promising material for this application. Making it possible to add value to the waste and reduce the operational cost of the treatment process.
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Palavras-chave
Rejeito, Minério, Foto-Fenton, Heterogêneo, Sulfonamidas, Waste, Iron mining, Photo-Fenton, Heterogeneous, Sulfonamides