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Neste trabalho foi investigado o uso de carvões activados para a remoção de paracetamol em meio aquoso, usando adsorventes disponíveis comercialmente, modificados quimicamente. Foi também usado um carvão obtido da activação de desperdícios de PET.A capacidade de adsorção dos carvões foi relacionada com as suas propriedades texturais e químicas. A natureza química dos materiais foi modificada por oxidação por via húmida A impregnação de ferro na superfície foi feita a partir de uma solução etanólica de nitrato de ferro. O objectivo deste trabalho consistiu assim em avaliar o efeito da alteração das propriedades superficiais na remoção do poluente alvo. A alteração da química superficial promovida pela oxidação mostrou-se determinante na capacidade de adsorção dos adsorventes modificados, assim como na velocidade de remoção de paracetamol. Os dados cinéticos foram ajustados aos modelos de pseudo-2ª ordem e de difusão intrapartícula e os parâmetros obtidos foram relacionados com as características texturais e químicas dos carvões activados. O efeito do ferro variou consoante o tipo de carvão usado nos ensaios cinéticos: no caso das amostras em pó, a presença de ferro aumentou a velocidade de remoção de paracetamol, ao contrário das amostras granulares, onde a velocidade diminuiu. Após oxidação a hidrofilicidade do carvão foi aumentada, o que favorece a transferência de moléculas de paracetamol para os poros do carvão (menor espessurada boundary layer). Ao mesmo tempo, a velocidade de adsorção e eficiência de remoção diminuem para o carvão oxidado, devido ao efeito competitivo das moléculas de água.
In this work the use of carbonaceous adsorbents for the removal of paracetamol, using commercially available adsorbents, and oxidized samples was investigated. An activated carbon nobtained from activation of PET was also used. The adsorption capacity of the adsorbents was linked to their textural and chemical features. The chemical nature of the as-received materials was modified by incorporating a transition metal (iron) on the carbon surface and by wet oxidation. The surface heterogeneity of the carbon created upon oxidation was found to be determinant in the adsorption capacity of the modified adsorbents, as well as on the rate of paracetamol removal. The experimental kinetic data was fitted to the pseudo-second order and intraparticle diffusion models and the parameters obtained were linked to the texturaland chemical features of the activated carbons. The effect of iron changed according to the carbon used in the kinetic studies: in the case of powdered samples, the presence of iron increased the rate of uptake of paracetamol, on the contrary of granular samples, where the rate decreased. After oxidation the wettability of the carbon was enhanced, which favors the transfer of paracetamol molecules to the pores of the carbon (smaller boundary layer thickness). At the same time, the overall adsorption rate and removal efficiency are reduced in the oxidized carbon, due to the competitive effect of water molecules.
In this work the use of carbonaceous adsorbents for the removal of paracetamol, using commercially available adsorbents, and oxidized samples was investigated. An activated carbon nobtained from activation of PET was also used. The adsorption capacity of the adsorbents was linked to their textural and chemical features. The chemical nature of the as-received materials was modified by incorporating a transition metal (iron) on the carbon surface and by wet oxidation. The surface heterogeneity of the carbon created upon oxidation was found to be determinant in the adsorption capacity of the modified adsorbents, as well as on the rate of paracetamol removal. The experimental kinetic data was fitted to the pseudo-second order and intraparticle diffusion models and the parameters obtained were linked to the texturaland chemical features of the activated carbons. The effect of iron changed according to the carbon used in the kinetic studies: in the case of powdered samples, the presence of iron increased the rate of uptake of paracetamol, on the contrary of granular samples, where the rate decreased. After oxidation the wettability of the carbon was enhanced, which favors the transfer of paracetamol molecules to the pores of the carbon (smaller boundary layer thickness). At the same time, the overall adsorption rate and removal efficiency are reduced in the oxidized carbon, due to the competitive effect of water molecules.
Descrição
Tese de mestrado, Química Tecnológica, Universidade de Lisboa, Faculdade de Ciências, 2009
Palavras-chave
Carvão activado Química de superfície Impregnação Cinética de adsorção Parecetamol Teses de mestrado - 2009
