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Previous issue date: 2016-08-04 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior - CAPES / The demand for electricity production, and the need for thermoelectric use as power generating units, makes it necessary to search for less polluting matrices. In this search the catalytic combustion of methane, both from natural gas and other sources (residue disposal, for example) have shown promising. It is known the use of cobalt oxides is an alternative to the use of catalysts based on noble metals which has shown high performance. In order to potentiate the activity of the cobalt based catalyst, thus reducing both the ignition temperature and the temperature of total burning of methane, this work proposes the production of cobalt-based precursors using different types of layered double hydroxides (LDHs).
Cobalt based catalysts partially substituted in layered double hydroxides (LDH Mg, Al and CO32-) were prepared by co-precipitation and impregnation with a nominal content of 9% CoII in LDH, or by impregnating a commercial hydrotalcite (HT). The LDH precursors were characterized by X-ray powder diffraction (XRD) and infrared absorption spectroscopy (FTIR). The XRD patterns indicated a LDH of 3R polytype. XRD showed the presence of Gibbisite in the HT precursor. The infrared spectra of precursor LDHs presented bands related to ?1, ?2 and ?3 vibrations of the carbonate anion, and interlayer water characteristic bands, thus in line with the XRD data. Analysis by XRD of the catalysts after calcination at 800 ?C showed the presence of periclase and spinel phases. Infrared spectra showed bands ascribed to the Mg-O and Co-O stretching in tetrahedral and octahedral sites as well as bands attributed to the Mg-O-Al bond and the cobalt spinel. The catalytic activity of these materials was investigated in the catalytic combustion of methane under kinetic regime, using predetermined reaction conditions to avoid diffusional limitations, resulting in a significant decrease in the combustion temperature, with the higher activity observed for the catalyst prepared by impregnating a commercial HT. Scanning electron microscopy (SEM) and quantitative chemical analysis (EDS) of catalysts with improved performance show both the homogeneous dispersion of the components in the sample surface and the higher aluminum content of the sample supported on HT. / A demanda de produ??o de energia el?trica, e a necessidade do uso de termel?tricas como unidades geradoras de energia, fazem com que seja necess?ria a busca por matrizes menos poluentes. Nessa busca a combust?o catal?tica do metano, tanto proveniente do g?s natural como de outras fontes (res?duo do tratamento de lixo, por exemplo), tem se mostrado promissora. Sabidamente o uso de ?xidos de cobalto ? uma alternativa, que vem mostrando alto desempenho, ao uso de catalisadores a base de metais nobres. Com o intuito de potencializar a atividade do catalisador a base de cobalto, reduzindo assim tanto a temperatura de igni??o quanto a de queima total do metano, esse trabalho prop?e sua produ??o utilizando como precursor diferentes tipos de hidr?xidos duplos lamelares (HDLs).
Catalisadores ? base de cobalto parcialmente substitu?dos em hidr?xidos duplos lamelares (HDL de Mg, Al e CO32-) foram preparados por co-precipita??o e impregna??o num teor nominal de 9% de CoII em HDL, ou por impregna??o em hidrotalcita comercial (HT). Os HDLs precursores foram caracterizados por difra??o de raios?X pelo m?todo de p? (DRX) e por espectroscopia de absor??o no infravermelho (FTIR). Os difratogramas indicaram a obten??o de um HDL de politipo 3R. Por meio do DRX foi identificada a presen?a de Gibbisita no suporte de HT. Os espectros de infravermelho dos HDLs precursores presentaram bandas referentes ?s vibra??es ?1, ?2 e ?3 do ?nion carbonato, al?m de bandas caracter?sticas de ?gua interlamelar, estando portanto de acordo com os dados de DRX. A an?lise por difra??o de raios-X dos catalisadores ap?s calcina??o a 800?C mostrou apenas as fases espin?lio e pericl?sio. Os espectros de infravermelho apresentaram bandas atribu?das aos estiramentos Mg?O e Co?O em s?tios tetra?dricos e octa?dricos, assim como bandas caracter?sticas de Mg?O?Al e de Co3O4. A atividade catal?tica desses materiais foi investigada na combust?o catal?tica do metano, em regime cin?tico, empregando-se condi??es reacionais preestabelecidas de forma a evitar limita??es difusionais, obtendo-se uma significativa diminui??o na temperatura de combust?o, sendo que a maior atividade foi observada para o catalisador preparado por impregna??o em HT comercial. Foi realizada microscopia eletr?nica de varredura (MEV) e an?lise qu?mica quantitativa (EDS) para os catalisadores com melhor desempenho, mostrando tanto a dispers?o homog?nea dos componentes na superf?cie das amostras como o maior teor de alum?nio presente na amostra suportada em HT.
| Identifer | oai:union.ndltd.org:IBICT/oai:localhost:jspui/1643 |
| Date | 04 August 2016 |
| Creators | Paiva, Maria Clara Adum de |
| Contributors | Herbst, Marcelo Hawrylak, Guedes, Guilherme pereira, Bigansolli, Antonio Renato |
| Publisher | Universidade Federal Rural do Rio de Janeiro, Programa de P?s-Gradua??o em Qu?mica, UFRRJ, Brasil, Instituto de Ci?ncias Exatas |
| Source Sets | IBICT Brazilian ETDs |
| Language | Portuguese |
| Detected Language | English |
| Type | info:eu-repo/semantics/publishedVersion, info:eu-repo/semantics/masterThesis |
| Format | application/pdf |
| Source | reponame:Biblioteca Digital de Teses e Dissertações da UFRRJ, instname:Universidade Federal Rural do Rio de Janeiro, instacron:UFRRJ |
| Rights | info:eu-repo/semantics/openAccess |
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