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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

SÃntese, caracterizaÃÃo e propriedades catalÃticas de sÃlidos mesoporosos: influÃncia da estrutura sobre a desativaÃÃo de catalizadores aplicados a reforma do metano / Synthesis, characterization and catalytic properties of mesoporous materials: influence of structure on disabling catalysts applied to reforming of methane

HÃlvio Silvester Andrade de Sousa 31 October 2012 (has links)
CoordenaÃÃo de AperfeiÃoamento de Pessoal de NÃvel Superior / Neste trabalho, aluminas mesoporosas dopadas com CeO2, MgO, ZrO2 ou La2O3 demonstraram que a estrutura dos sÃlidos influenciou no comportamento de desativaÃÃo de catalisadores na reforma seca do metano. Os sÃlidos foram caracterizados atravÃs de difraÃÃo de raios-X, anÃlise quÃmica, espectroscopia Raman, reduÃÃo termoprogramada, anÃlises texturais e termogravimÃtrica, microscopia eletrÃnica de transmissÃo e alta resoluÃÃo, antes e apÃs os testes catalÃticos. NÃquel, platina ou rutÃnio foram dispersos sobre os suportes porosos CeO2-Al2O3, ZrO2-Al2O3, MgO-Al2O3 e La2O3-Al2O3, formando distintas fases. Os catalisadores contendo rutÃnio ou platina foram em geral mais ativos na reforma seca do metano quando comparados aqueles contendo nÃquel, devido a maior dispersÃo das espÃcies de PtOx ou Ruo dispersas sobre MgAl2O4 ou CeAlO3. A resistÃncia à degradaÃÃo fÃsica dos sÃlidos contendo platina ou rutÃnio conduziu a um efeito do promotor para a formaÃÃo de espÃcies de carbono lÃbeis. Sobre o catalisador Ru/MgO-Al2O3, as nanopartÃculas de Ruo dispersas em MgAl2O4 foram mais acessÃveis as molÃculas de metano e diÃxido de carbono, apesar de serem as fontes para a formaÃÃo de carbono amorfo, grafite e nanotubos de carbono. / Mesoporous alumina doped with CeO2, MgO, ZrO2 or La2O3 demonstrated that the solid structure influenced on the deactivation behaviour of the catalysts in dry reforming of methane. Solids were characterized by X-ray diffraction, chemical analysis, Raman spectroscopy, termoprogrammed reduction, textural and thermogravimetric analyses and transmission electron microscopy, before and after the catalytic test. Nickel, ruthenium or platinum dispersed on porous CeO2-Al2O3, ZrO2-Al2O3, MgO-Al2O3 and La2O3-Al2O3 resulted in the formation of distinct phases. Catalysts possessing ruthenium or platinum were more active than the nickel counterparts due to the better dispersion of PtOx or Ruo on MgAl2O4 and CeAlO3 phases. The elevated resistance of ruthenium or platinum against physical degradation led to a promoting effect to labile carbon formation. Over Ru/MgO-Al2O3 catalyst, Ruo nanoparticles dispersed on MgAl2O4 were almost certainly accessible to methane and carbon dioxide molecules and the source supporting for the formation of such amorphous reactive carbon, graphite and carbon nanotubes, as well.

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