Avalia??o da dessulfuriza??o de diesel utilizando adsorventes mesoporosos modificados p?s-situ com ?ons met?licos

Autor: Sales, Rafael Viana
Jazyk: portugalština
Rok vydání: 2015
Předmět:
Zdroj: Repositório Institucional da UFRNUniversidade Federal do Rio Grande do NorteUFRN.
Druh dokumentu: masterThesis
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A emiss?o de compostos sulfurados provenientes da queima de combust?veis derivados do refino do petr?leo, como ?leo diesel e gasolina, ? respons?vel por ocasionar danos ambientais, ? sa?de humana e aumento de custos industriais. Neste trabalho, foram estudados processos adsortivos de compostos sulfurados do diesel proveniente da Refinaria Potiguar Clara Camar?o, RPCC, com elevado teor de enxofre, utilizando s?licas mesoporosas do tipo MCM-41, que foram obtidas por m?todo hidrot?rmico, a partir de duas s?licas amorfas, s?lica MP1, novo material avaliado neste trabalho e uma s?lica comercial, utilizada para compara??o. Para os adsorventes mesoporosos MCM-41, sintetizados, foi avaliada a capacidade de adsor??o de enxofre em colunas de leito fixo e, posteriormente, os mesmos foram modificados, p?s-situ, com c?tions met?licos por impregna??o ?mida e dispers?o f?sica. Diferentes composi??es qu?micas dos compostos met?licos foram testadas, com a utiliza??o de ?xidos e sais, para a obten??o de s?tios ativos e avalia??o da complexa??o, entre o enxofre dos compostos org?nicos e os c?tions met?licos inseridos nos adsorventes, favorecendo a adsor??o. Os adsorventes sintetizados, puros e modificados, foram caracterizados atrav?s das t?cnicas de difratometria de raios X - DRX, espectroscopia de infravermelho com transformada de Fourier - FTIR, an?lises termogravim?tricas - TG/DTG, an?lises texturais pelo m?todo de BET/BJH e microscopia eletr?nica de varredura ? MEV com espectroscopia de energia dispersiva (EDS). Um planejamento fatorial do tipo 23, foi aplicado para o estudo do processo de adsor??o onde blends dos c?tions met?licos foram testados na adsor??o dos compostos sulfurados existentes. O monitoramento do teor de enxofre no diesel, durante o processo de adsor??o, ocorreu por t?cnica de Espectrometria de Fluoresc?ncia na Regi?o do Ultravioleta (FUV). A cin?tica e o equil?brio de adsor??o foram avaliados, onde isotermas de equil?brio foram obtidas para a avalia??o da capacidade m?xima de adsor??o de compostos sulfurados, nos sistemas adsorventes desenvolvidos neste trabalho. Foram obtidas capacidades m?ximas de adsor??o, em mg.g-1, de 16,64 e 14,98, respectivamente, para os adsorventes testados: 2AgS/MCM-41(M) e 1NiS1AgS/MCM-41(M). Os dados experimentais foram ajustados aos modelos de equil?brio de Langmuir e Freundlich. A remo??o de enxofre presente no diesel foi significante, atingindo o m?ximo de adsor??o de 94,9%, em rela??o ? concentra??o inicial deste contaminante. Atrav?s do estudo estat?stico, constatou-se que os blends preparados a partir dos adsorventes modificados por sais apresentaram uma capacidade de adsor??o maior em rela??o aos preparados por impregna??o de ?xidos met?licos, o que pode contribuir para a redu??o de custos industriais, uma vez que o m?todo de impregna??o ?mida dispensa uma segunda calcina??o.
The emission of sulfur compounds from the burning of oil products, such as diesel and gasoline, is responsible for causing environmental damage to human health and increase industrial costs. In this work, adsorptive processes of sulfur compounds from the diesel provided by the refinery Potiguar Clara Camar?o, RPCC, with high sulfur content, were studied using MCM-41 type of mesoporous silica which were obtained by hydrothermal method, from two amorphous silicas, MP1 silica, a new material evaluated in this work and a commercial silica, used for comparison. For MCM-41 mesoporous adsorbents, synthesized, it was evaluated the capability of sulfur adsorption in fixed bed columns, and later they were modified post-situ with metal cations by wet impregnation and physical dispersion. Different chemical compositions of metal compounds were tested with the use of oxides and salts, to obtain active sites and evaluation of complexing, between the sulfur of organic compounds and the metal cations inserted on the adsorbent, favoring adsorption. The synthesized adsorbents, pure and modified, were characterized by the techniques of X-ray diffraction - XRD, Fourier transform infrared spectroscopy - FTIR, thermogravimetric analysis - TG / DTG, textural analysis by the method of BET / BJH and scanning electron microscopy - SEM with energy dispersive spectroscopy (EDS). A 23 factorial plan was applied to study the adsorption process which metal cations blends were tested in the adsorption of existing sulfur compounds. The sulfur content monitoring in diesel fuel during the adsorption process occurred by ultraviolet fluorescence Spectrometry (UVF). The adsorption kinetics and equilibrium were evaluated, where equilibrium isotherms were obtained for the evaluation of the maximum adsorption capacity of sulfur compounds in adsorbent systems developed in this work. Maximum adsorption capacities were obtained, at mg.g-1, 16,64 and 14,98, respectively, for the tested adsorbent: 2AgS/MCM-41(M) e 1NiS1AgS/MCM-41(M. The experimental data were fit to a Langmuir balance models and Freundlich. The removal of sulfur present in the diesel was significant, ranging from 54.3% to 88.9% compared to the initial concentration of contaminant. By statistical analysis it was found that blends prepared from the adsorbent modified by salts showed a higher adsorption capacity than the ones prepared by impregnation of metal oxides, which may contribute to the reduction of industrial costs, since the wet impregnation method dispenses a second calcination.
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