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Page de résumé pour ULgetd-04082009-092228

Auteur : Greisch, Jean-François
E-mail de l'auteur : jfgreisch@ulg.ac.be
URN : ULgetd-04082009-092228
Langue : Anglais/English
Titre : Development and Characterization of Fullerene Based Molecular Systems using Mass Spectrometry and Related Techniques.
Intitulé du diplôme : Doctorat en sciences de l'ingénieur
Département : FSA - Département de chimie appliquée
Jury :
Nom : Titre :
CAMPBELL, Eleanor E. B. Membre du jury/Committee Member
DREWELLO, Thomas Membre du jury/Committee Member
LEYH, Bernard Membre du jury/Committee Member
MARIEN, José Membre du jury/Committee Member
PIRARD, Jean-Paul Membre du jury/Committee Member
Remacle, Françoise Membre du jury/Committee Member
Crine, Michel Président du jury/Committee Chair
DE PAUW, Edwin Promoteur/Director
Mots-clés :
  • Spectrométrie de masse/ Mass Spectrometry
  • Fullerènes & dérivatives/ Fullerene derivatives
  • Hydrogénisation & Déshydrogénisation des fullerènes/fullerene hydrogenation and dehydrogenation
  • Mobilité ionique/Ion mobility.
  • Complexes de cyclodextrines/Cyclodextrin complexes
Date de soutenance : 2008-10-27
Type d'accès : Public/Internet
Résumé :

The investigation and control of the properties of carbon based materials such as fullerenes

and nanotubes is a highly dynamic research field. Due to its unique properties, e.g. an almost nano-dimensional size, three-dimensional cage topology, hydrophobicity, rich redox- and photochemistry, large absorption cross section, … C60 has a high potential as building block for molecular devices and biological applications. It can be functionalized, anchored to a surface and self-assembled into larger supramolecular entities, such as monolayers. Mass

spectrometry and related techniques such as ion-molecule reactions, action spectroscopy and ion mobility have been used throughout this work to study fullerene based systems, ranging from hydrides, derivatives, non-covalent complexes and coordinated metal complexes.

Simulations predicting structural, electronic and mechanical properties have been combined with the experimental results to assist in their analysis and interpretation. Using ion molecule reactions, the reactivity of gas phase C60 anions with methanol has been studied. Hydride formation by simple collisions in the gas phase with methanol as well as reversible

dehydrogenation by infrared multiphoton activation has been demonstrated. C60

functionalization by 3’-azido-3’-deoxythymidine (AZT) has been performed and the charged product characterized both by collisional activation and action spectroscopy. Deprotonation has been shown to lead to rearrangements of the nucleoside analogue and to a subsequent charge transfer to the fullerene. To prevent unwanted rearrangements and side reactions,

encapsulation of C60 is suggested, the host molecule acting as a steric barrier.

C60 complexation by γ-cyclodextrins has been performed and the ions of the complexes characterized both by collisional activation and ion mobility. It has been demonstrated that,

compared to deprotonated species, the sodiated C60:(γ-cyclodextrin)2 ions were highly compact structures.

With only two small polar caps accessible to reagents, sodiated C60:

(γ-cyclodextrin)2 complexes sterically protect the C60 core from unwanted side reactions.

Finally, explorative work on C60 immobilization on silver colloids using surface enhanced Raman spectroscopy and on the characterization of C60 complexes with iron and manganese

porphyrin is presented.

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