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Thèse de Doctorat
DOI
10.11606/T.46.2010.tde-21072010-083127
Document
Auteur
Nom complet
Vitor Hugo Soares de Melo
Adresse Mail
Unité de l'USP
Domain de Connaissance
Date de Soutenance
Editeur
São Paulo, 2010
Directeur
Jury
Toma, Henrique Eisi (Président)
Ferreira, Ana Maria da Costa
Gonçalves, Norberto Sanches
Oliveira, Luiz Fernando Cappa de
Santos, Paulo Sergio
Titre en portugais
Investigação por meio de efeito SERS e SERRS dos sistemas híbridos formados pela interação da 3,6-bi-2-piridil-1,2,4,5-tetrazina e complexos de rutênio com ouro macroscópico e nanoparticulado
Mots-clés en portugais
Complexos binucleares
Efeito SERS
Hot spots
Mecanismo químico
Nanopartículas de ouro
Sistemas híbridos
Resumé en portugais
A síntese e caracterização de sistemas hetero-híbridos gerados a partir da 3,6-bi-2-piridil-1,2,4,5-tetrazina (bptz) e interações com ouro nanoparticulado são abordados nesta tese. O bptz foi estudado por meio de métodos espectroscópicos e teóricos, focalizando principalmente o efeito SERS associado à adsorção em nanopartículas de ouro. O mecanismo de transferência de carga para metais macroscópicos foi transposto para a condição nanoparticulada, envolvendo ligações químicas entre bptz e as nanopartículas. Os complexos estudados possuem fórmula geral [LmRu(µ-bptz)RuLm]Xn, com “L” indicando os ligantes periféricos 5-cloro-1,10-fenantrolina (Clphen) ou 4’-(fenil)-2,2’:6’,2”-terpirdina (ptpy) e “X” os contra-íons. Foram investigadas suas espectroeletroquímicas eletrônica e SERS, e as mudanças de perfil vibracional foram modeladas, incorporando o mecanismo de transferências de carga entre complexo e o ouro, além dos mecanismos ressonantes e eletromagnéticos
Titre en anglais
Investigation of SERS and SERRS effect of the Hybrid Systems made by the interaction of 3,6-bi-2-pyridyl-1,2,4,5-tetrazine and its ruthenium complexes with macroscopic and nanoparticle gold
Mots-clés en anglais
Binuclear complexes
Chemical mechanism
Gold nanoparticles
Hot spots
Hybrid systems
SERS Effect
Resumé en anglais
The synthesis and investigation of heterohybrid systems encompassing 3,6-bi-2-pyridyl-1,2,4,5-tetrazine (bptz) and its ruthenium complexes associated with gold nanoparticles are dealt with in this thesis. Bptz was characterized by spectroscopic and theoretical techniques, focusing on its SERS spectra after the adsorption onto nanoparticles. The charge transfer mechanism in the SERS spectra of macroscopic metals was transposed to the nanoparticle condition, assuming the formation of chemical bonds between bptz and the nanoparticles. Complexes of general formula [LmRu(µ--bptz)RuLm]Xn, “L” the peripheric ligants 5-chlorine-1,10-phenantroline or 4’-(phenyl)-2,2’:6’,2”-terpyrdine (ptpy), and “X” counter-ions were also investigated, with special emphasis on their electronic and SERS spectroelectrochemistry. The changes in the vibrational profiles were successfully explained by the occurrence of charge transfer between the adsorbed complex and gold, in addition to the electromagnetic and resonance mechanisms.
 
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Date de Publication
2010-08-17
 
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Centro de Informática de São Carlos
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