Made available in DSpace on 2014-12-17T15:41:57Z (GMT). No. of bitstreams: 1 VitorRMM_DISSERT.pdf: 2544703 bytes, checksum: 4453e8b3e10e994e669daf77efdaa72b (MD5) Previous issue date: 2012-08-04 / Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico / Perovskites oxides win importance by its properties and commercials applications, they have a high thermal stability, have conductive properties, electrical, catalytic, electro catalytic, optical and magnetic, and are thermally stable. Because of these properties, are being widely studied as carriers of oxygen in the process of power generation with CO2 capture. In this work, the base carrier system La1-xMexNiO3 (Me = Ca and Sr) were synthesized by the method via the combustion reaction assisted by microwave. were synthesized from the combustion reaction method by microwave process. This method control the synthesi`s conditions to obtain materials with specific characteristics. The carriers calcined at 800 ? C/2h were analyzed by thermal analysis (TG-DTA), to verify its thermal stability, X-ray diffraction (XRD) to verify the phase formation, with subsequent refinement by the Rietveld method, to quantify the percentage of phases formed, the surface area by BET method was determined, scanning electron microscopy (SEM) was obtained to evaluate the material morphology and temperature programmed reduction (TPR) was done to observe the metallic phase of the nickel. After all proposed characterization and analysis of their results can be inferred to these oxides, key features so that they can be applied as carriers for combustion reactions in chemical cycles. The final products showed perovskite-type structures K2NiF4 (main) and ABO3. / ?xidos com estrutura tipo perovsquita destacam-se por suas diversas propriedades e aplica??es comerciais, pois possuem alta estabilidade t?rmica, apresentam propriedades condutoras, el?tricas, catal?ticas, eletrocatal?ticas, ?pticas e magn?ticas, al?m de serem termicamente est?veis. Devido a estas propriedades, est?o sendo amplamente estudados como carreadores de oxig?nio em processos de gera??o de energia com captura de CO2. Neste trabalho, carreadores a base do sistema La1-xMexNiO3 ( Me = Ca e Sr) foram sintetizados a partir do m?todo via rea??o de combust?o assistida por microondas. Este m?todo controla as condi??es de s?ntese para obten??o de materiais com caracter?sticas espec?ficas. Os carreadores calcinados a 800?C/2h foram analisados atrav?s de an?lise t?rmica (TG-DTA), para verifica??o de sua estabilidade t?rmica; difra??o de raios-X (DRX), para verifica??o das fases formadas, com posterior refinamento atrav?s do m?todo de Rietveld, para quantificar o percentual das fases formadas; ?rea superficial pelo m?todo BET; microscopia eletr?nica de varredura (MEV) e redu??o ? temperatura programada (TPR). Ap?s toda caracteriza??o proposta e an?lise dos seus resultados pode-se inferir a esses ?xidos, caracter?sticas fundamentais para que os mesmos possam ser aplicados como carreadores em rea??es de combust?o por ciclos qu?micos. Os carreadores de oxig?nio obtidos possuem estruturas perovsquitas do tipo K2NiF4 (principal) e ABO3.

Submitted by Automa??o e Estat?stica (sst@bczm.ufrn.br) on 2016-02-29T21:50:23Z No. of bitstreams: 1 JoseAntonioBarrosLealReisAlves_TESE.pdf: 5550413 bytes, checksum: 4c1d98761f0c020539c60eca7d324bf6 (MD5) / Approved for entry into archive by Arlan Eloi Leite Silva (eloihistoriador@yahoo.com.br) on 2016-03-01T21:55:58Z (GMT) No. of bitstreams: 1 JoseAntonioBarrosLealReisAlves_TESE.pdf: 5550413 bytes, checksum: 4c1d98761f0c020539c60eca7d324bf6 (MD5) / Made available in DSpace on 2016-03-01T21:55:58Z (GMT). No. of bitstreams: 1 JoseAntonioBarrosLealReisAlves_TESE.pdf: 5550413 bytes, checksum: 4c1d98761f0c020539c60eca7d324bf6 (MD5) Previous issue date: 2014-06-09 / O aumento da demanda energ?tica est? sendo atendida em grande parte por reservas de combust?veis f?sseis, que emitem CO2, SOx e v?rios outros gases poluentes. Cresce tamb?m a busca por combust?veis que emitam menos poluentes e que possuam a mesma efici?ncia energ?tica. Neste contexto, o hidrog?nio (H2) vem sendo cada vez mais reconhecido como um potencial carreador de energia para um futuro pr?ximo. Isso ocorre porque o H2 pode ser obtido por diversas rotas e tem uma vasta ?rea de aplica??o, al?m de possuir queima limpa, gerando apenas H2O como produto da queima, e a maior densidade de energia por unidade de massa. O processo de reforma com recircula??o qu?mica (RRQ) vem sendo bastante investigado nos ?ltimos anos, pois ? poss?vel regenerar o carreador de oxig?nio por meio da aplica??o de ciclos de redu??o e oxida??o. Este trabalho tem como objetivo geral desenvolver carreadores de oxig?nio a base de n?quel e cobalto para estudar a reatividade em processo de reforma com recircula??o qu?mica. Os carreadores de oxig?nio foram preparados por tr?s m?todos diferentes: combust?o assistida por microondas, impregna??o por via ?mida e coprecipita??o. Todos os materiais sintetizados possuem a mesma quantidade em massa das fases ativas (60%m/m). Os 40%m/m restantes s?o de La2O3 (8%m/m), Al2O3 (30%m/m) e MgO (2%). Os carreadores de oxig?nio foram nomeados da seguinte forma: N ou C, n?quel ou cobalto, seguido do n?mero 3 ou 6, que significa 30 ou 60% de fase ativa na forma de ?xido e C, CI ou CP, que significa combust?o assistida por micro-ondas, combust?o assistida por micro-ondas seguida de impregna??o por via ?mida e co-precipita??o. Os carreadores de oxig?nio foram ent?o caracterizados atrav?s das t?cnicas de difra??o de raios X (DRX), ?rea espec?fica (BET), redu??o ? temperatura programada (RTP) e microscopia eletr?nica de varredura (MEV). Os resultados de caracteriza??o mostraram que os diferentes m?todos de s?ntese levaram ? obten??o de diferentes estruturas e morfologias. Os testes de redu??o/oxida??o utilizando CH4 como redutor e ar sint?tico como oxidante foram realizados com os carreadores de oxig?nio N6C e C6C, N6CI e C6CI e N6CP e C6CP. Os testes revelaram diferentes comportamentos e que estes dependem do tipo de fase ativa bem como do tipo de s?ntese. O carreador de oxig?nio N6C foi o que produziu mais H2, ao passo que o carreador de oxig?nio C6CI foi o que produziu mais CO2 e H2O, sem ocorr?ncia da forma??o de coque. / Increasing energy demand is being met largely by fossil fuel reserves, which emit CO2, SOx gases and various other pollutants. So does the search for fuels that emit fewer pollutants and have the same energy efficiency. In this context, hydrogen (H2) has been increasingly recognized as a potential carrier of energy for the near future. This is because the H2 can be obtained by different routes and has a wide application area , in addition to having clean burning, generating only H2O as a product of combustion , and higher energy density per unit mass . The Chemical Looping Reforming process (CLR) has been extensively investigated in recent years, it is possible to regenerate the catalyst by applying cycles of reduction and oxidation. This work has as main objective to develop catalysts based on nickel and cobalt to study the reactivity of reform with chemical recycling process. The catalysts were prepared by three different methods: combustion assisted by microwave, wet impregnation and co-precipitation. All catalysts synthesized have the same amount by weight of the active phases (60% w / w). The other 40 % m/m consists in La2O3 (8% w / w), Al2O3 (30% w / w) and MgO (2%). Oxygen carriers have been named as follows: N or C, nickel or cobalt, followed by the number 3 or 6, meaning 30 to 60% of active phase in the oxide form and C, CI or CP, which means self-combustion assisted by microwave, self-combustion assisted by microwave followed by wet impregnation and co-precipitation. The oxygen carriers were then characterized by the techniques of X-ray diffraction (XRD), surface area (BET), temperature programmed reduction (TPR) and scanning electron microscopy (SEM). The characterization results showed that the different synthesis methods have led to obtaining different morphologies and structures. Redox tests using CH4 as reducing agent and sintetic air as oxidant agent was done with N6C and C6C, N6CI and C6CI and N6CP and C6CP oxygen carriers. The tests revealed different behaviors, depending on active phase and on synthesis procedure. N6C oxygen carrier produced high levels of H2. The C6CI oxygen carrier produced CO2 and H2O without carbon deposits.