Made available in DSpace on 2014-12-17T15:41:53Z (GMT). No. of bitstreams: 1 RicardoMO_DISSERT.pdf: 2015893 bytes, checksum: dea62cb9390752fd7430293c73c9a1dd (MD5) Previous issue date: 2011-12-06 / Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico / The catalytic cracking of triglycerides presents itself as a possible alternative to the production of biofuels with low emission of pollutants. In this work were synthesized the SAPO-5, the catalysts for the cracking reaction of soybean oil is presented. The solids were powder X-ray diffraction (XRD), thermogravimetric analysis (TG/DTG) and infrared spectroscopy (FTIR). The analyses indicated that the synthesis method has employed to obtain materials with high surface area and high acid. The soybean oil thermal and thermal catalytic cracking, realized from the room temperature to 450 ?C in a simple distillation system, has allowed obtaining two liquid fractions, each consisting of two phases, one aqueous and another organic, organic liquid (OL). The OL obtained from first fractions has shown high acid index, even in the thermal catalytic process. The products obtained in the cracking of soybean oil were analyzed by distillation, acid number, infra-red spectroscopy, density, viscosity, carbon residue, cetane number determination and characterization. The analysis of the products obtained in the presence and in the absence of the SAPO-5 permitted to conclude that all the solids tested presented catalytic activity in the deoxygenation of final products only at the second step of the cracking process / O craqueamento catal?tico de triacilglicer?deos se apresenta como uma alternativa vi?vel para a produ??o de biocombust?veis com baixa emiss?o de poluentes. Neste trabalho foi sintetizado o SAPO-5, o catalisador foi utilizado na rea??o de craqueamento do ?leo de Girassol. O s?lido foi caracterizado por difra??o de raios -X, an?lise termogravim?trica, espectroscopia no infravermelho. As an?lises indicaram que atrav?s do m?todo de s?ntese empregado foram obtidos materiais com elevada ?rea espec?fica e alta acidez. A partir do craqueamento t?rmico e termocatal?tico do ?leo de girassol, realizado desde a temperatura ambiente at? 450 oC em um sistema de destila??o simples, foram obtidas duas fra??es l?quidas, cada uma contendo duas fases, uma aquosa e outra org?nica. A primeira fra??o do l?quido org?nico obtido apresentou alto ?ndice de acidez, no processo de craqueamento t?rmico. Os produtos obtidos no craqueamento de ?leo de Girassol foram analisados por destila??o, ?ndice de acidez, espectroscopia no infravermelho, densidade, viscosidade e determina??o do ?ndice de cetano. A an?lise dos produtos obtidos na presen?a e na aus?ncia do SAPO-5, sintetizados permitiu concluir que todos os s?lidos testados apresentaram atividade catal?tica para a desoxigena??o dos produtos finais apenas na segunda etapa do processo de craqueamento

Made available in DSpace on 2014-12-17T15:42:16Z (GMT). No. of bitstreams: 1 LuizaPFCG_TESE.pdf: 3362653 bytes, checksum: 0de0a428d24980a5f9b2bf94d2e9214f (MD5) Previous issue date: 2012-08-23 / To overcome the challenge of meeting growing energy demand in a sustainable way, biodiesel has shown very promising as alternative energy can replace fossil fuels, even partially. Industrially, the biodiesel is produced by homogeneous transesterification reaction of vegetable oils in the presence of basic species used as catalysts. However, this process is the need for purification of the esters obtained and the removal of glycerin formed after the reaction. This context, the alternative catalysts have that can improve the process of biodiesel production, aiming to reduce costs and facilitate its production. In this study, the AlSBA-15 support with Si / Al ratio = 50 was synthesized, as like as the heterogeneous catalysts of zinc oxide and magnesium supported on mesoporous AlSBA-15 silica, in the concentrations of 5, 10, 15 and 30 %, relative to the support. The textural properties and structural characterization of catalysts and supports were determined by techniques: X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) coupled to the chemical analyzer, adsorption / desorption of N2, thermal analysis (TG / DTG), absorption spectroscopy in the infrared (FTIR) and X-ray photoelectron spectroscopy (XPS). Characterization results indicated that the support AlSBA-15 retained the hexagonal ordered after the incorporation of zinc oxide and magnesium oxide in the holder. For heterogeneous catalysts, ZnO-AlSBA-15, that was observed the presence of zinc oxide nanoparticles dispersed in the surface and interior channels of the mesoporous and microporous support. The catalytic activity was evaluated by the transesterification reaction of sunflower oil via methylic route, and some reaction parameters were optimized with the most active catalyst in biodiesel production by sunflower oil. For the series of heterogeneous catalysts, the sample with 30 % ZnO supported on AlSBA-15 showed a better conversion of triglyceride to methyl esters, about 95.41 % of reaction conditions: temperature 175 ?C, with molar ratio of 42:1, stirring at 200 rpm and under a pressure of 14 bar for 6 h. The catalyst MgO-AlSBA-15 showed no catalytic activity in the studied reactions / Para superar o desafio de atender a crescente demanda por energia de forma sustent?vel, o biodiesel tem se demonstrado bastante promissor como alternativa energ?tica, que possa substituir os combust?veis fosseis, mesmo que parcialmente. Industrialmente, o biodiesel ? produzido atrav?s de rea??o homog?nea de transesterifica??o de ?leos vegetais na presen?a de esp?cies b?sicas utilizadas como catalisadores. Entretanto, este processo h? a necessidade de purifica??o dos ?steres obtidos e a remo??o da glicerina formada ap?s a rea??o. Diante deste contexto, tem-se buscado catalisadores alternativos, que possa aprimorar o processo de produ??o de biodiesel, visando diminuir os custos e facilitar a sua produ??o. Neste trabalho, foram sintetizados o suporte AlSBA-15 na raz?o Si/Al = 50, e os catalisadores heterog?neos de ?xido de zinco e de magn?sio suportado sobre s?lica mesoporosa AlSBA-15, nas concentra??o de 5, 10, 15 e 30 %, com rela??o ao suporte. As propriedades texturais e a caracteriza??o estrutural dos catalisadores e do suporte foram determinadas pelas t?cnicas de: difratometria de raios X (DRX), microscopia eletr?nica de varredura (MEV), microscopia eletr?nica de transmiss?o (MET) acoplada ao analisador qu?mico, adsor??o/dessor??o de N2, an?lise t?rmica (TG/DTG), espectroscopia de absor??o na regi?o do infravermelho (FTIR) e espectroscopia fotoeletr?nica de raios X (XPS). Os resultados de caracteriza??o indicaram que o suporte AlSBA-15 preservou a estrutura hexagonal ordenada, ap?s a incorpora??o do ?xido de zinco e do ?xido de magn?sio no suporte. Em rela??o aos catalisadores heterog?neos, ZnO-AlSBA-15, observou-se a presen?a de nanopart?culas de ?xido de zinco dispersas na superf?cie e no interior dos canais microporosos e mesoporosos do suporte. A atividade catal?tica foi avaliada pela rea??o de transesterifica??o do ?leo de girassol via rota met?lica, e alguns par?metros reacionais foram otimizados com o catalisador mais ativo na produ??o de biodiesel pelo ?leo de girassol. Para as s?ries de catalisadores heterog?neos, a amostra com 30 % ZnO suportado na AlSBA-15 apresentou melhor convers?o dos triglicer?deos em ?steres met?licos, cerca de 95,41 %, nas condi??es reacional de: temperatura de 175 ?C, com raz?o molar de 42:1, em agita??o de 200 rpm e sob press?o de 14 bar durante 6 h. O catalisador MgO-AlSBA-15 n?o apresentou atividade catal?tica nas rea??es estudadas

Submitted by Ricardo Cedraz Duque Moliterno (ricardo.moliterno@uefs.br) on 2015-10-01T23:29:45Z No. of bitstreams: 1 Aspergillus terreus isolamento identifica??o e avalia??o da capacidade catalitica na redu??o de cetonas pr? quirais.pdf: 1820055 bytes, checksum: c5c60d2c4b1c577c84c8b1baaa95660d (MD5) / Made available in DSpace on 2015-10-01T23:29:45Z (GMT). No. of bitstreams: 1 Aspergillus terreus isolamento identifica??o e avalia??o da capacidade catalitica na redu??o de cetonas pr? quirais.pdf: 1820055 bytes, checksum: c5c60d2c4b1c577c84c8b1baaa95660d (MD5) Previous issue date: 2014-09-30 / The object of this inquiry is the isolation, the selection and the potential evaluation of a microorganism with biocatalytic activity in carrying out selective-stereo biorreduction of pro-chial ketones. In the research procedure, Fungi was isolated from soil samples contaminated with lead. Only one of the isolates fungi, identified as Aspergillus terreus, presented good catalytic activity in the reduction of acetophenone. The biomass was grown submerged in broth culture, inoculated with 1,1 x 103 (spores/mL of malt extract) and maintained at 30?C under orbital agitation. Morphological differences and catalytic activity were evaluated in function of the orbit of agitation during the growth process. The catalytic activity in terms of conversion of acetophenone and enantiomeric excess (S), ee_S, in 1-feniletanol, was determinate in conjunction with the growth curve of the fungus. The results were used to construct a graphic showing the variation of quality of the catalyst, according to age of biomass. Apart from acetophenone were tested o-Xacetophenone, p-Xacetophenone and m-Xacetophenone (X = methyl, methoxy, nitro, fluorine, bromine). For reaction with 24 hours growing cells (30?C; 150rpm/r = 50mm), the conversions were between 27% and 97% with ee_S between 41% and 83%. For reactions with cells in suspension in buffered medium (pH = 4.5 ? 6,5) was decrease in activity/selectivity at pH above 5.5. The kinetics of conversion was evaluated for biomasses with different ages and for various concentrations of acetophenone. An amount between 100mg and 200mg of biomass (dry mass) with 168 hours of culture can convert 100mg of acetophenone to 1(S)-feniletanou ee_S (91%) with 98% yield in 72 hours of reaction (93% at 48 hours). The development of this process described above, constitutes the body of this thesis. / O objetivo desta pesquisa ? o isolamento, a sele??o e a avalia??o de um microorganismo com atividade biocatalisadora na biorredu??o estereoseletiva de cetonas pro-quirais. No procedimento de investiga??o, fungos foram isolados de amostras de solo contaminadas com chumbo. Apenas um dos fungos isolados, identificado geneticamente como Aspergillus terreus, apresentou boa atividade catal?tica na redu??o de acetofenona. A biomassa foi cultivada submersa no caldo de cultura, inoculado com 1,1x103 (esporos/mL de extrato de malte) e mantido a 30? sob agita??o orbital. Diferen?as morfol?gicas e de atividade catal?tica foram avaliadas em fun??o da ?rbita de agita??o durante o crescimento. A atividade catal?tica, em termos de convers?o da acetofenona e do excesso enantiom?rico (S), ee_S, no 1-feniletanol, foi determinada em conjunto com a curva de crescimento do fungo. Os resultados foram usados para construir um gr?fico mostrando a varia??o da qualidade do catalisador em fun??o da idade da biomassa. Al?m de acetofenona, foram testadas o-Xacetofenona, p-Xacetofenona e m-Xacetofenona (X=metil, metoxi, nitro, fl?or, bromo). Para 24 horas de rea??o com c?lulas em crescimento (30?C; 150rpm/r = 50mm), as convers?es ficaram entre 94 e 100%, com ee_S ? 98% para acetofenona e para acetofenonas orta ou meta substitu?das. Com substituintes na posi??o para, a convers?o ficou entre 27% e 97%, com ee_S entre 41% e 83%. Para rea??es com c?lulas em suspens?o em meio tamponado (pH = 4,5 ? 6,5), houve queda na atividade/seletividade em pH acima de 5,5. A cin?tica de convers?o foi avaliada para biomassas com idades distintas e para v?rias concentra??es de acetofenona. Uma quantidade entre 100mg e 200mg de biomassa (massa seca) com 168 horas de cultura, pode converter 100mg de acetofenona a 1(S)-feniletanol (ee_S 91%), com 98% de rendimento em 72 horas de rea??o (93% em 48 horas). O desenvolvimento desse processo, acima descrito, constitui o corpo desta Tese.

Submitted by Automa??o e Estat?stica (sst@bczm.ufrn.br) on 2017-06-13T19:56:34Z No. of bitstreams: 1 LarissaCiciannyLuzFerreiraDeAraujo_TESE.pdf: 3361603 bytes, checksum: 8da0327f1fa708d7b02bec63cf53a5f0 (MD5) / Approved for entry into archive by Arlan Eloi Leite Silva (eloihistoriador@yahoo.com.br) on 2017-06-19T11:40:01Z (GMT) No. of bitstreams: 1 LarissaCiciannyLuzFerreiraDeAraujo_TESE.pdf: 3361603 bytes, checksum: 8da0327f1fa708d7b02bec63cf53a5f0 (MD5) / Made available in DSpace on 2017-06-19T11:40:01Z (GMT). No. of bitstreams: 1 LarissaCiciannyLuzFerreiraDeAraujo_TESE.pdf: 3361603 bytes, checksum: 8da0327f1fa708d7b02bec63cf53a5f0 (MD5) Previous issue date: 2016-08-26 / Os nanomateriais (catalisadores) mesoporosos e microporosos s?o considerados promissores para obten??o de derivados leves a partir de fra??es pesadas do petr?leo e como adsorventes para prote??o ambiental. Este trabalho reportou a sintetize pelo m?todo hidrot?rmico, e caracteriza??o de catalisadores heterog?neos mesoporosos, do tipo SBA-15, com adi??o dos metais c?rio e alum?nio, avaliando sua atividade e seletividade na degrada??o t?rmica de ?leo pesado. As amostras dos materiais nanoestruturados foram caracterizadas por an?lise termogravim?trica (TG/DTG), difra??o de raios X (DRX), microscopia eletr?nica de varredura (MEV), espectroscopia de fluoresc?ncia de raios X (FRX), espectroscopia de absor??o na regi?o do infravermelho com transformada de Fourier (FTIR) e adsor??o de nitrog?nio (BET). A caracteriza??o mostrou que os materiais sintetizados resultaram em um catalisador nanoestruturado, ordenado e com di?metro de poros e ?rea superficial de acordo com a literatura existente. Com o intuito de verificar a atividade catal?tica dos mesmos, utilizou-se uma amostra de petr?leo pesado (?API=14), fornecido pela Petrobras, realizando-se atrav?s da termogravimetria o processo de degrada??o t?rmica e catal?tica do ?leo. Mediante as curvas termogravim?tricas obtidas, observou-se uma redu??o na temperatura de in?cio do processo de decomposi??o catal?tica do petr?leo. Atrav?s do modelo cin?tico n?o isot?rmico de Ozawa Flynn Wall (OFW) obtiveram-se alguns par?metros para determina??o da energia de ativa??o aparente das decomposi??es. Os resultados obtidos das difra??es de raio X mostraram atrav?s de picos caracter?sticos que a estrutura hexagonal foi formada, verificando que a melhor raz?o foi Si/Ce = 5 devido a sua intensidade em alto ?ngulo. Os espectros de infravermelho apresentaram absor??es caracter?sticas de materiais da fam?lia SBA-15. Da adsor??o de nitrog?nio, obtendo-se par?metros compat?veis aos encontrados na literatura, que lhes conferem serem promissores na ?rea da degrada??o de petr?leo, devido aos seus mesoporos facilitarem o acesso de grandes mol?culas. O di?metro m?dio dos poros variou significativamente com a incorpora??o do alum?nio e do c?rio. A espessuras de parede (Wt) ficou na faixa de 2,96 a 4,07 nm, observando assim um aumento deste par?metro que deve-se a incorpora??o dos metais na parede, indicando que a incorpora??o do c?rio, n?o bloqueou os mesoporos. O acr?scimo de alum?nio reduziu a area superficial (SBET) de 893 para 763 m2g-1, no entanto com o acr?scimo do c?rio com o alum?nio esta ?rea aumentou para 826 m2g-1. Para o petr?leo a temperatura inicial e final de perda de massa; apresentando apenas dois eventos devido ao teor de enxofre mercapt?dico, o qual influencia no surgimento do terceiro evento, j? que esse teor ? medido pela quantidade de enxofre nos an?is arom?ticos (HC pesados). A mistura do Petr?leo + 12% de Ce5Al50SBA-15 evidenciando a atividade catal?tica deste material. / Nanomaterials (catalysts) are microporous and mesoporous considered promising for obtaining light oil products from heavy oil fractions and adsorbents for environmental protection. This paper reported the synthesizes by hydrothermal method, and characterization of mesoporous heterogeneous catalysts, the SBA-15 type with addition of metals cerium and aluminum, evaluating their activity and selectivity in the thermal degradation of heavy oil. Samples of nanostructured materials were characterized by thermal gravimetric analysis (TG / DTG), X-ray diffraction (XRD), scanning electron microscopy (SEM), ray fluorescence spectroscopy X (XRF) spectroscopy, absorption in the infrared region Fourier transform (FTIR) and nitrogen adsorption (BET). The characterization showed that the synthesized materials resulted in a nanostructured catalyst and ordered pore diameter and surface area according to the literature. In order to check the catalytic activity of the same, we used a heavy oil sample (?API = 14), supplied by Petrobras, is performing through thermogravimetry the process of thermal and catalytic degradation of the oil. Through the thermogravimetric curves, it was observed a reduction in the opening of oil decomposition catalytic process temperature. Through non isothermal kinetic model Ozawa Flynn Wall (OFW) gave some parameters to determine the apparent activation energy of decomposition. Obtaining as results of X-ray diffraction showed through characteristic peaks that the hexagonal structure was formed, noting that the best reason was Si / Ce = 5 because of its intensity at a high angle. The infrared spectra showed absorptions family material characteristics SBA-15. The nitrogen adsorption, obtaining parameters compatible with those found in the literature which confer them to be promising in the field of oil degradation due to their mesopores facilitate access of large molecules. The average pore diameter varied significantly with the incorporation of aluminum and cerium. The wall thickness (Wt) was in the range from 2.96 to 4.07 nm, thus observing an increase in this parameter which is due to incorporation of the metals into the wall, indicating that the incorporation of cerium, did not block the mesopores. The addition of aluminum reduced the surface area (SBET) of 893 to 763 m2 g-1, however with the addition of cerium with aluminum this area increased to 826 m2 g-1. For the oil temperature and the initial end of weight loss; presenting only two events due to mercapt?dico sulfur, which influences the appearance of the third event, since that content is measured by the amount of sulfur in aromatic rings (heavy HC). The mixture of oil + 12% of Ce5Al50SBA-15 showing the catalytic activity of this material.

Made available in DSpace on 2014-12-17T14:07:00Z (GMT). No. of bitstreams: 1 AuristelaCM_DISSERT.pdf: 1278248 bytes, checksum: cbdcf9cab5a2fc14113da4b21bc60b64 (MD5) Previous issue date: 2011-11-28 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / The mesoporous molecular sieves of the MCM-41 and FeMCM-41 type are considered promissory as support for metals used as catalysts in oil-based materials refine processes and as adsorbents for environmental protection proposes. In this work MCM-41 and FeMCM41 were synthesized using rice husk ash - RHA as alternative to the conventional silica source. Hydrothermal synthesis was the method chosen to prepare the materials. Pre-defined synthesis parameters were 100?C for 168 hours, later the precursor was calcinated at 550?C for 2 hours under nitrogen and air flow. The sieves containing different proportions of iron were produced by two routes: introduction of iron salt direct synthesis; and a modification post synthesis consisting in iron salt 1 % and 5% impregnation in the material followed by thermal decomposition. The molecular sieves were characterized by X ray diffraction XRD, Fourier transform infrared spectroscopy FT-IR, X ray fluorescence spectroscopy XFR, scanning electronic microscopy SEM, specific surface area using the BET method, Termogravimetry TG. The kinetic model of Flynn Wall was used with the aim of determining the apparent activation energy of the surfactant remove (CTMABr) in the MCM- 41 porous. The analysis made possible the morphology characterization, identifying the presence of hexagonal structure typical for mesoporous materials, as well as observation of the MCM41 and iron of characteristic bands. / As peneiras moleculares mesoporosas do tipo MCM-41 e FeMCM-41, s?o consideradas promissoras como suporte para metais, usadas como catalisadores em processos de refino de materiais a base de petr?leo e como adsorventes com o prop?sito de prote??o ambiental. Neste trabalho MCM-41 e FeMCM-41 foram sintetizadas utilizando a cinza da casca de arroz CCA, como alternativa para a fonte de s?lica. O m?todo escolhido foi a s?ntese hidrotermal para o preparo dos materiais, a temperatura de 100 ?C por 168 horas em estufa, posteriormente foi calcinado a 550 ?C por 2 horas sob fluxo de nitrog?nio e ar. As peneiras moleculares contendo diferentes propor??es de ferro foram produzidas por duas rotas: introdu??o do sal de ferro no gel de s?ntese e impregna??o de 1% e 5% de ferro no MCM-41 sintetizado. As peneiras moleculares foram caracterizadas por difra??o de raios X DRX, espectroscopia no infravermelho por transformada de Fourier (Fourier transform infrared spectroscopy FT-IR), espectroscopia de fluoresc?ncia de raios X FRX, microscopia eletr?nica de varredura MEV, ?rea superficial espec?fica atrav?s do m?todo BET e Termogravimetria TG. O modelo cin?tico de Flynn Wall foi utilizado com o objetivo de determinar a energia de ativa??o aparente da remo??o do surfactante (CTMABr) nos poros do MCM-41. As an?lises possibilitaram a caracteriza??o morfol?gica, identificando a presen?a da estrutura hexagonal t?pica dos materiais mesoporosos, assim como das bandas caracter?sticas do MCM41 e do ferro.

Made available in DSpace on 2014-12-17T15:42:28Z (GMT). No. of bitstreams: 1 MariaJFC_TESE.pdf: 4007652 bytes, checksum: 7bb363c54641679d79bbff5c76de539f (MD5) Previous issue date: 2013-06-03 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / The processing of heavy oil produced in Brazil is an emergency action and a strategic plan to obtain self-sufficiency and economic surpluses. Seen in these terms, it is indispensable to invest in research to obtain new catalysts for obtaining light fraction of hydrocarbons from heavy fractions of petroleum. This dissertation for the degree of Doctor of Philosophy reports the materials preparation that combine the high catalytic activity of zeolites with the greater accessibility of the mesoporosity, more particularly the HZSM-5/MCM-41 hybrid, done by synthesis processes with less environmental impact than conventional ones. Innovative methodologies were developed for the synthesis of micro-mesoporous hybrid material by dual templating mechanism and from crystalline zeolitic aluminosilicate in the absence of organic template. The synthesis of hybrid with pore bimodal distribution took place from one-single organic directing agent aimed to eliminate the use of organic templates, acids of any kind or organic solvents like templating agent of crystalline zeolitic aluminosilicate together with temperature-programmed microwave-assisted, making the experimental procedures of preparation most practical and easy, with good reproducibility and low cost. The study about crystalline zeolitic aluminosilicate in the absence of organic template, especially MFI type, is based on use of H2O and Na+ cation playing a structural directing role in place of an organic template. Advanced characterization techniques such as X-Ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM), Highresolution Transmission Electron Microscopy (HRTEM), Adsorption of N2 and CO2, kinetic studies by Thermogravimetric Analysis (TGA) and Pyrolysis coupled to Gas Chromatography/Mass Spectrometry (Pyrolysis-GC/MS) were employed in order to evaluate the synthesized materials. Achieve the proposed objectives, has made available a set of new methodologies for the synthesis of zeolite and hybrid micro-mesoporous material, these suitable for catalytic pyrolysis of heavy oils aimed at producing light fraction / O processamento do petr?leo pesado produzido no Pa?s ? uma a??o emergencial e estrat?gica para obter a auto-sufici?ncia e super?vits econ?micos. Neste sentido, ? indispens?vel o investimento em pesquisas de novos catalisadores para obten??o de derivados leves a partir de fra??es pesadas do petr?leo. O trabalho de doutorado aqui reportado dedicouse ? prepara??o de materiais que combinem, numa ?nica estrutura, a elevada atividade catal?tica de ze?litas, com melhor acessibilidade de materiais mesoporosos, como a estrutura h?brida HZSM-5/MCM-41, utilizando processos de s?ntese com menor impacto ambiental que os convencionais. Metodologias inovadoras foram desenvolvidas para a s?ntese do catalisador h?brido micro-mesoporoso ou ze?lito-mesoporoso por mecanismo de direcionamento estrutural via duplo agente diretor org?nico e tamb?m a partir de estrutura zeol?tica sintetizada na aus?ncia total de direcionador org?nico. Esse ?ltimo, tamb?m chamado de s?ntese do h?brido com distribui??o bimodal de poros a partir de um ?nico agente diretor org?nico, visou eliminar o uso dos direcionadores org?nicos, ?cidos de qualquer natureza ou solventes org?nicos como molde estrutural da estrutura zeol?tica em conjunto com o m?todo hidrot?rmico assistido por irradia??o via micro-ondas, tornando o procedimento experimental de prepara??o pr?tico e simples, com boa reprodutibilidade e menor custo. A metodologia de prepara??o da ze?lita MFI do tipo ZSM-5 utiliza H2O e c?tions Na+ no papel de direcionamento estrutural e compensa??o de cargas na estrutura. T?cnicas relevantes de caracteriza??o, como Difra??o de Raios-X (XRD), Espectroscopia no Infravermelho com Transformada de Fourier (FTIR), Microscopia Eletr?nica de Varredura (SEM), Microscopia Eletr?nica de Transmiss?o de Alta Resolu??o (HRTEM), Adsor??o de N2 e CO2, estudos cin?ticos via An?lises Termogravim?tricas (TGA) e Pir?lise acoplada ? Cromatografia Gasosa/Espectrometria de Massas (Pyrolysis-GC/MS), foram empregadas no intuito de avaliar os materiais sintetizados. Alcan?ados os objetivos propostos, disponibilizou-se um conjunto de novas metodologias para s?ntese de catalisadores zeol?ticos e h?bridos micromesoporosos, estes adequados para pir?lise catal?tica de ?leos pesados visando ? produ??o de derivados leves

Made available in DSpace on 2014-12-17T15:41:45Z (GMT). No. of bitstreams: 1 MariaJFCpdf.pdf: 4931245 bytes, checksum: 45a7ea893d17f478c73adf56787579aa (MD5) Previous issue date: 2008-12-22 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / The present work reports the study of nanoporous structures, aiming at their use in research directed to the current demand of the petroleum industry to value heavy oil. Initially, two ways were chosen for the synthesis of porous structures from the molecular sieves of type Si-MCM-41. In the first way, the structure MCM-41 is precursory for heteroatom substitutes of silicon, generating catalyst of the type Al-MCM-41 from two different methods of incorporation of the metal. This variation of the incorporation method of Aluminum in the structure of Si-MCM-41 was carried out through the conventional procedure, where the aluminum source was incorporated to the gel of synthesis, and the procedure post-synthesis, where the Aluminum source was incorporated in catalyst after the synthesis of Si-MCM-41. In the second way, the MCM-41 acts as a support for growth of nanocrystals of zeolite embedded in their mesoporous, resulting in hybrid MCM-41/ZSM-5 catalyst. A comparative analysis was carried through characterizations by XRD, FTIR, measures of acidity through n-butylamine adsorption for TGA, SEM-XRF and N2 adsorption. Also crystalline aluminosilicate with zeolitic structure MFI of type ZSM-5 was synthesized without using organic templates. Methodologies to the preparation of these materials are related by literature using conventionally reactants that supply oxides of necessary silicon and aluminum, as well as a template agent, and in some cases co-template. The search for new routes of preparation for the ZSM-5 aimed at, above all, the optimization of the same as for the time and the temperature of synthesis, and mainly the elimination of the use of organic templates, that are material of high cost and generally very toxic. The current study is based on the use of the H2O and Na+ cations playing the role of structural template and charge compensation in the structure. Characterizations by XRD, FTIR, SEM-XRF and N2 adsorption were also conducted for this material in order to compare the samples of ZSM-5 synthesized in the absence of template and those used industrially and synthesized using structuring / O presente trabalho relata o estudo de estruturas nanoporosas, visando o uso em pesquisas que atendam a atual demanda da ind?stria do petr?leo, de valorizar ?leos pesados. Inicialmente, optou-se por duas vertentes para a s?ntese de estruturas porosas a partir da peneira molecular do tipo Si-MCM-41. Na primeira vertente, a estrutura MCM-41 ? precursora para hetero?tomos substituintes do sil?cio, gerando catalisadores do tipo Al-MCM-41 a partir de dois diferentes m?todos de incorpora??o do metal. Essa varia??o do m?todo de incorpora??o do Alum?nio na estrutura do Si-MCM-41 se deu atrav?s do procedimento convencional, no qual a fonte de alum?nio foi incorporada ao gel de s?ntese e do procedimento p?s-s?ntese, no qual a fonte de Alum?nio foi incorporada ao catalisador ap?s a s?ntese do Si-MCM-41. Na segunda vertente, o MCM-41 age como suporte para o crescimento de nanocristais de ze?lita embutidos nos seus mesoporos, resultando no catalisador h?brido MCM-41/ZSM-5. Uma an?lise comparativa foi realizada atrav?s de caracteriza??es por XRD, FTIR, medidas de acidez atrav?s de dessor??o de n-butilamina por TGA, SEM-XRF e Adsor??o de N2. Tamb?m foi sintetizado um aluminossilicato cristalino com estrutura zeol?tica MFI do tipo ZSM-5, na aus?ncia total de direcionador org?nico. Metodologias relacionadas ? prepara??o desses materiais s?o relatadas pela literatura utilizando-se convencionalmente reagentes que forne?am os ?xidos de sil?cio e de alum?nio necess?rios, bem como um agente direcionador, e em alguns casos at? co-direcionadores. A busca por novas rotas de prepara??o para a ZSM-5 visou, sobretudo, a otimiza??o da mesma no que se refere ao tempo e ? temperatura de s?ntese, e principalmente a elimina??o do uso dos direcionadores org?nicos, que s?o materiais de alto custo e geralmente muito t?xicos. O atual estudo se baseia na utiliza??o da H2O e dos c?tions Na+ desempenhando o papel de direcionamento estrutural e compensa??o de cargas na estrutura. Caracteriza??es por XRD, FTIR, SEM-XRF e Adsor??o de N2 tamb?m foram realizadas para esse material, a fim de comparar as amostras de ZSM-5 sintetizadas na aus?ncia do direcionador e aquelas utilizadas industrialmente e sintetizadas utilizando estruturantes