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?xidos estruturados do tipo perovsquita para gera??o de g?s de s?ntese via reforma a seco de metanoSilva, Elania Maria Fernandes 25 July 2017 (has links)
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Previous issue date: 2017-07-25 / Catalisadores de alto desempenho v?m sendo bastante investigados com o objetivo de aumentar o rendimento dos processos de reforma a seco do metano (RSM). Alguns metais de transi??o, em especial o n?quel, s?o amplamente estudados para essa aplica??o. Por possu?rem propriedades catal?ticas, estabilidade t?rmica e qu?mica, os ?xidos com estrutura do tipo perovsquita s?o materiais promissores como precursores catal?ticos em processos de RSM. O objetivo deste estudo ? avaliar a efici?ncia de ?xidos do tipo perovsquita como catalisadores m?ssicos e como suportes catal?ticos na reforma a seco de metano (RSM). Assim, ?xidos tipo perovsquita ABO3 foram sintetizados pelo m?todo de combust?o assistida por micro-ondas usando ureia como combust?vel. Os materiais foram calcinados a 900 ?C por 2h. Ap?s a calcina??o todos os ?xidos preparados foram impregnados com 20 % (m/m) de n?quel e calcinados novamente a 600 ?C por 2h. As amostras foram caracterizadas por: difra??o de raios X (DRX), redu??o ? temperatura programada (RTP) e microscopia eletr?nica de varredura com espectroscopia de energia dispersiva (MEV-EDS). Testes de reforma de metano com CO2 foram realizados para avalia??o desses materiais como catalisadores na produ??o de g?s de s?ntese. Ap?s os testes de reforma, os catalisadores foram submetidos novamente a caracteriza??es para investiga??o da exist?ncia de carbono nas superf?cies dos ?xidos. De acordo com os difratogramas de raios X, fases secund?rias de ?xidos de n?quel foram formadas ap?s a impregna??o do n?quel nos p?s. Os mapeamentos obtidos atrav?s de EDS mostraram que a metodologia de impregna??o resultou numa dispers?o homog?nea das part?culas de ?xido de n?quel na superf?cie das perovsquitas. Os testes catal?ticos foram realizados a 750 ?C durante 10 horas. Os catalisadores avaliados apresentaram melhores desempenhos, tanto de convers?es como de estabilidade, ap?s a impregna??o de n?quel, mostrando que as perovsquitas podem ser potenciais suportes catal?ticos para reforma a seco do metano. / High-performance catalysts have been widely researched in order to increase the yield in methane dry reforming processes (DRM). Some transition metals, especially nickel, are largely studied for this purpose. Due to its catalysts? properties, thermal and chemical stability, perovskite-type oxides ABO3 are promising materials as catalytic precursors in DRM processes. The objective of this study is to evaluate the efficiency of perovskite type oxides as catalysts and as supports in dry reforming of methane (DRM). Perovskite-type oxides ABO3 were synthesized by microwave assisted combustion using urea as fuel and calcinated at 900 ?C for 2h. After the calcination, all the prepared oxides were impregnated with 20% (w/w) of nickel and calcinated again at 600?C for 2h. The samples were characterized by the following techniques: x-ray diffraction (XRD), temperature programmed reduction (TPR), and dispersive energy scanning electron microscopy with energy dispersive spectroscopy (SEM-EDS). Methane reforming tests with CO2 were performed for evaluation of these materials as catalysts in the production of syngas. After the reforming tests, the catalysts were submitted once again to characterizations for the evaluation of the existence of carbon in the oxides? surface. According to the X-ray diffractograms, secondary phases of nickel oxides were formed after the nickel impregnation in the powders. The mapping by EDS showed that the impregnation methodology resulted in a homogeneous dispersion of the nickel oxide particles on the perovskite?s surface. The catalytic tests were performed at 750 ? C for 10 hours. The catalysts showed better performances, conversions and stability, after nickel impregnation, showing that the perovskites may be potential catalytic supports for dry reforming methane.
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