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Doctoral Thesis
DOI
https://doi.org/10.11606/T.75.2007.tde-27032008-084800
Document
Author
Full name
Flávio Colmati Junior
E-mail
Institute/School/College
Knowledge Area
Date of Defense
Published
São Carlos, 2007
Supervisor
Committee
Gonzalez, Ernesto Rafael (President)
Albuquerque, Hamilton Brandão Varela de
Linardi, Marcelo
Olivi, Paulo
Perez, Joelma
Title in Portuguese
Estudo de catalisadores de Pt-Sn para o ânodo da célula a combustível de membrana trocadora de prótons alimentada com etanol direto
Keywords in Portuguese
células a combustível
DEFC
Pt-Sn
Abstract in Portuguese
Eletrocatalisadores de Pt-Sn suportados em carbono de elevada área superficial foram preparados por redução química de precursores metálicosm em solução usando como agente redutor o ácido fórmico. Esse método mostrou-se muito eficiente sendo possível obter tanto catalisadores com baixos teores de Sn (razão atômica Pt:Sn de 9:1) como com altos teores de Sn (razão atômica Pt:Sn de 1:3). Entretanto, apesar de ser o Sn reduzido e ancorado sobre o substrato de carbono apenas parte deste Sn é inserido na rede cristalina da Pt sendo necessário um tratamento térmico em atmosfera redutora para aumentar o grau de liga. Foram realizados tratamentos térmicos entre 100 e 500 ºC e o melhor desempenho na célula a combustível foi obtido com o material Pt3Sn tratado a 200 ºC. O tratamento térmico a 200ºC permitiu um incremento no grau de liga dos metais Pt e Sn sem modificar a estrutura cúbica de face centrada da Pt e sem promover a coalescência das nanopartículas ancoradas no suporte de carbono. Os materiais de Pt-Sn foram caracterizados através de difração de raios-X, absorção de raios-X e microscopia eletrônica de transmissão. A atividade para a eletro-oxidação de etanol foi avaliada através de técnicas eletroquímicas e experimentos em células a combustível unitárias. Para complementar o estudo da eletro-oxidação de etanol foram realizados estudos fundamentais usando monocristais de Pt com baixos e altos índices de Miller.
Title in English
Study of Pt-Sn electrocatalysts for the anodes of proton exhange membrane fuel cell supplied with ethanol
Keywords in English
DEFC
fuel cell
Pt-Sn
Abstract in English
Carbon supported Pt-Sn catalysts were prepared by reduction of Pt and Sn precursors with formic acid. The method allowed the efficient preparation of catalysts with low Sn contents (Pt:Sn ratio 9:1) and with high Sn contents (Pt:Sn ratio 1:3. In spite of the fact that Sn was anchored in the material, only part of the Sn is inserted in the fcc structure of Pt. Therefore, a thermal treatment in a reducing atmosphere was necessary to increase the degree of alloy. Thermal treatments were done between 100 and 500 oC and the Pt3Sn material treated at 200 oC showed the best performance in a direct ethanol fuel cell. The thermal treatment at 200 oC allowed an increase of the degree of alloy without modifying the face centered cubic Pt structure and without promoting the coalescence of the nanoparticles anchored on the carbon support. The Pt-Sn catalysts were characterized by X-ray diffraction, X-ray absorption and transmission electron microscopy. The activity for the electro-oxidation of ethanol was evaluated with electrochemical techniques and experiments in a single direct ethanol fuel cell. Studies with Pt single crystals with low and high Miller indices were done to complement the study of the ethanol electro-oxidation.
 
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Publishing Date
2008-03-31
 
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