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Doctoral Thesis
DOI
10.11606/T.46.2009.tde-29092009-101645
Document
Author
Full name
Marcio Yuji Matsumoto
E-mail
Institute/School/College
Knowledge Area
Date of Defense
Published
São Paulo, 2009
Supervisor
Committee
Toma, Henrique Eisi (President)
Angnes, Lúcio
Espósito, Breno Pannia
Mayer, Ildemar
Nunes, Genebaldo Sales
Title in Portuguese
Desenvolvimento da química supramolecular de porfirazinas polimetaladas
Keywords in Portuguese
Dispositivos moleculares
Eletrocatálise
Fullereno
Porfirazina
Química supramolecular
Rutênio
Abstract in Portuguese
Nesta tese foram perseguidos novos avanços no campo das tetrapiridilporfirazinas supramoleculares polimetaladas, visando explorar a maior capacidade de conjugação eletrônica esperada para essa classe de compostos, e seus reflexos nas propriedades eletrônicas e eletroquímicas. Foram apresentadas novas rotas sintéticas para obtenção de tetra(3,4-piridil)porfirazinas centrometaladas coordenadas a complexos polipiridínicos de rutênio, MTRPyPz (M = Cu, Co). As propriedades espectroscópicas e eletroquímicas foram investigadas com o auxílio de técnicas de espectroscopia UV-Vis, Raman ressonante, voltametria cíclica, espectroeletroquímica e espectrometria de massas. Foram desenvolvidas aplicações em dispositivos amperométricos para determinação eletrocatalítica de substratos importantes nas indústrias, como nitrito, sulfito e ácido ascórbico. Os estudos também abrangeram a formação de compósitos das porfirazinas tetrarrutenadas com fullereno. Os nanomateriais híbridos apresentaram uma alta eficiência nos processos eletrocatalíticos com menor sobrepotencial no eletrodo, abrindo perspectivas interessantes de utilização em dispositivos moleculares
Title in English
Supramolecular chemistry of polymetallic porphyrazines
Keywords in English
Electrocatalysis
Fullerene
Molecular devices
Porphyrazine
Ruthenium
Supramolecular chemistry
Abstract in English
Research in supramolecular polymetallic tetrapyridylporphyrazines has been pursued in this Thesis, aiming the exploitation of the favorable electronic delocalization associated with conjugated aromatic rings, and its influence on the electronic and electrochemical properties. New synthetic routes have been developed for the preparation of tetra(3,4-pyridyl)porphyrazines containing Cu(II) and Co(II) ions in the center, and four chlorobis(2,2´bipyridine)ruthenium(II) complexes attached to the peripheral pyridyl groups. Their spectroscopic and electrochemical behaviors were investigated by means of UV-Vis and resonance Raman spectroscopy, cyclic voltammetry, spectroelectrochemistry and mass spectrometry. Applications in amperometric devices for determination of nitrite, sulfite and ascorbic acid were successfully developed. The thesis also focused on nanocomposites generated from the polymetallic porphyrazines and fullerene (C60). Such hybrid nanomaterials exhibited enhanced electrocatalytic activity associates with a significant decrease of overpotential, opening exciting perspectives of use in molecular devices
 
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Publishing Date
2009-12-08
 
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