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A presente dissertação teve como principal objetivo a contribuição para o desenvolvimento do projeto Oxi-E3D, que consiste na otimização de um processo avançado, o processo eletroquímico 3D, para a remoção dos fármacos carbamazepina (CBZ) e diclofenac (DCF) com vista à sua aplicação no tratamento de águas residuais. No processo eletroquímico 2D foram utilizados como elétrodos, um ânodo (boron doped diamond (BDD) ou titânio revestido com óxido de irídio e rutênio (MMO)) e um cátodo (aço inoxidável ou carbon felt). No processo eletroquímico 3D, que inclui o uso de um terceiro elétrodo particulado, foram usados como adsorventes, um biochar com diferentes granulometrias (1-2 mm e (1-2 mm e <75 µm) e um carvão ativado granulado comercial da marca Saratech®. As melhores condições de trabalho para os ensaios 2D da CBZ foram as seguintes: distância entre elétrodos 7,5 cm, elétrodos titânio vs aço inoxidável, concentração da solução de CBZ 10 mg/L, pH 7 e solução de cloreto de sódio 0,1 mol/L como eletrólito, as quais permitiram obter uma eficiência de remoção de 54,2% ao fim de 10 min de reação. Relativamente ao processo com o DCF, as condições de trabalho mais favoráveis foram as seguintes: distância entre elétrodos 7,5 cm, conjunto de elétrodos titânio vs aço inoxidável, concentração da solução de DCF 10 mg/L, pH 7 e solução de cloreto de sódio 0,02 mol/L como eletrólito, com as quais se conseguiu obter uma eficiência de remoção de 58,6% ao fim de 10 min de reação.
No processo eletroquímico 3D para a CBZ e para o DCF, foram usadas as mesmas condições de trabalho que nos ensaios 2D. Em relação à CBZ, o adsorvente que apresentou melhor desempenho foi o biochar 1-2 mm (saturado) com uma eficiência de remoção de 99,8% ao fim de 5 min e para o DCF, foi o biochar (saturado) com granulometria inferior a 75 µm que apresentou a melhor eficiência de remoção, 86,1% para 10 minutos de reação. Os resultados alcançados referentes à remoção dos fármacos CBZ e DCF, que apresentam respetivamente carga neutra e negativa, são promissores para a aplicação do processo eletroquímico 3D no tratamento de águas residuais urbanas.
The main objective of this dissertation was to contribute to the development of the oxi-e3d project, which consists of the optimization of an advanced process, the 3d electrochemical process, for the removal of the pharmaceuticals carbamazepine (cbz) and diclofenac (dcf) with a view to its application in wastewater treatment. In the 2d electrochemical process, an anode (diamond doped with boron (bdd) or titanium coated with iridium and ruthenium oxide (mmo)) and a cathode (stainless steel or carbon felt) were used as electrodes. In the 3d electrochemical process, which includes the use of a third particulate electrode, a biochar with different particle sizes (1-2 mm and <75 μm) and a commercial granular activated carbon from saratech® were used as adsorbents. The best working conditions for the 2d tests of cbz were as follows: distance between electrodes 7.5 cm, titanium vs stainless steel electrodes, concentration of cbz solution 10 mg/l, ph 7 and sodium chloride solution 0.1 mol/l as electrolyte, which allowed to obtain a removal efficiency of 54.2% after 10 min of reaction. Regarding the process with dcf, the most favorable working conditions were as follows: distance between electrodes 7.5 cm, set of titanium vs stainless steel electrodes, concentration of dcf solution 10 mg/l, ph 7 and sodium chloride solution 0.02 mol/l as electrolyte, which allowed to achieve a removal rate of 58.6% after 10 min of reaction. In the 3d electrochemical process for the cbz and for the dcf, the same working conditions of the 2d tests were used. Regarding the cbz, the adsorbent with the best performance was the 1-2 mm biochar (saturated) with an efficiency removal of 99,8% after 5 min reaction time, and for dcf, it was the biochar (saturated) with a particle size of less than 75 μm that presented the best removal efficiency, 86.1% after 10 min reaction time. The results achieved regarding the removal of the pharmaceuticals cbz and dcf, which have neutral and negative charge, respectively, are promising for the application of the 3d electrochemical process in the treatment of urban wastewaters.
The main objective of this dissertation was to contribute to the development of the oxi-e3d project, which consists of the optimization of an advanced process, the 3d electrochemical process, for the removal of the pharmaceuticals carbamazepine (cbz) and diclofenac (dcf) with a view to its application in wastewater treatment. In the 2d electrochemical process, an anode (diamond doped with boron (bdd) or titanium coated with iridium and ruthenium oxide (mmo)) and a cathode (stainless steel or carbon felt) were used as electrodes. In the 3d electrochemical process, which includes the use of a third particulate electrode, a biochar with different particle sizes (1-2 mm and <75 μm) and a commercial granular activated carbon from saratech® were used as adsorbents. The best working conditions for the 2d tests of cbz were as follows: distance between electrodes 7.5 cm, titanium vs stainless steel electrodes, concentration of cbz solution 10 mg/l, ph 7 and sodium chloride solution 0.1 mol/l as electrolyte, which allowed to obtain a removal efficiency of 54.2% after 10 min of reaction. Regarding the process with dcf, the most favorable working conditions were as follows: distance between electrodes 7.5 cm, set of titanium vs stainless steel electrodes, concentration of dcf solution 10 mg/l, ph 7 and sodium chloride solution 0.02 mol/l as electrolyte, which allowed to achieve a removal rate of 58.6% after 10 min of reaction. In the 3d electrochemical process for the cbz and for the dcf, the same working conditions of the 2d tests were used. Regarding the cbz, the adsorbent with the best performance was the 1-2 mm biochar (saturated) with an efficiency removal of 99,8% after 5 min reaction time, and for dcf, it was the biochar (saturated) with a particle size of less than 75 μm that presented the best removal efficiency, 86.1% after 10 min reaction time. The results achieved regarding the removal of the pharmaceuticals cbz and dcf, which have neutral and negative charge, respectively, are promising for the application of the 3d electrochemical process in the treatment of urban wastewaters.
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Keywords
Carbamazepina Diclofenac Processo eletroquímico 3D Biochar Carvão ativado Carbamazepine 3d electrochemical process Activated carbon