Redução do Oxigênio Molecular por [Fe(Bipy)3]/C: influência do suporte e do tratamento térmico na atividade catalítica.

• Ano de defesa: 2011
• Autor(a) principal: Rêgo, Ulisses Alves do
• Orientador(a): BEZERRA, Cícero Wellington Brito
• Tipo de documento: Dissertação
• Tipo de acesso: Acesso aberto
• Idioma: por
• Instituição de defesa: Universidade Federal do Maranhão
• Programa de Pós-Graduação: PROGRAMA DE PÓS-GRADUAÇÃO EM QUÍMICA/CCET
• Departamento: DEPARTAMENTO DE TECNOLOGIA QUÍMICA/CCET
• País: Brasil
• Palavras-chave em Português: Célula a Combustível; Redução de Oxigênio; Eletrocatálise; Oxygen Reduction; Electrocatalysis; Fuel Cells
• Área do conhecimento CNPq: Química Analítica
• Link de acesso: http://tedebc.ufma.br:8080/jspui/handle/tede/1560

This work consisted in the preparation and study of catalytic activity for reduction of molecular oxygen (ROM) based on head-treated coordination compounds with nitrogenated ligands, impregnated on carbon nanosupports (nanotube - NTC, and nanoparticles - Vulcan). The following ions complexes [Fe(bipy)3]2+ and [Fe(TPTZ)2]2+ (2,2 '-bipyridine and 2 ,4,6-tris (2-pyridyl) -1,3,5-triazine) were synthesized and characterized in solution (electron spectroscopy in the region UV-vis, cyclic voltammetry). The following materials were prepared C1: Fe(10%)-Bipy/NTC; C2: Fe(5%) -Bipy/NTC; C3: Fe(5%)-Bipy/Vulcan and C4: Fe(5%)-TPTZ/Vulcan. The comparison between C1 and C2, and between C2 and C3 materials, showed, respectively, the effect of metal loading and the nature of the carbon support on their catalytic efficiency. The comparison among all and C4 (already reported in the literature) allowed the verification of experimental methodology employed. The effect of temperature on the electrocatalytic performance was observed for C1. The following pyrolysis temperatures were used: 600-1000 oC. The results showed that metal loading and the nature of the support influence the catalytic ability of the materials. The best pyrolysis temperature observed to generate active sites in C1 for the ROM was at 800 oC. All materials were treated at this temperature, and the efficiency order observed was: C4 (Fe (5%) -TPTZ/Vulcan) >> C1 (Fe(10%)-Bipy/NTC) > C2 (Fe(5%)-Bipy/NTC) > C3 (Fe (5%) -Bipy/Vulcan). For not heat treated materials, the activity order observed was: C3 (Fe(5%)-Bipy/Vulcan) C4 (Fe (5%)-TPTZ/Vulcan) > C1 (Fe (10%)-bipy/NTC) > C2 (Fe (5%) -Bipy/NTC). C2 and C3 catalysts showed a tendency to reduce the molecular oxygen according to 2e- mechanism, while C1 and C4 materials by 4e- mechanism. For some reason, the TPTZ ligand favored the generation of catalytic sites more efficient than Bipy in these materials.