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Séparation de charges de molécules linéaires insérées dans des zéolithes à canaux

Abstract : Sorption of anthracene and Diphenyl-polyene (trans-Stilbene, 1,4-Diphenyl-1,3-butadiene, 1,6-Diphenyl-1,3,5-hexatriene) in channel type zeolite such as Ferrierite (M-FER), ZSM-5 (MnZSM-5) and Mordenite (M-MOR) was studied by Monte Carlo simulations, diffuse reflectance UV-visible spectroscopy, Raman scattering and Electron Spin Resonance (ESR). Theoretical and experimental results provide evidence of the adsorption of molecules into the channel of the zeolite. For polarizing cation (M = H+ et Li+) spontaneous ionization induces the formation of a long-lived radical cation – electron pair. During the charge recombination electron-hole pairs are identified by pulsed ESR techniques. In case of molecules adsorbed without any chemical modification (M = Na+, K+, Rb+, Cs+) laser UV flash photolysis give rise to radical pairs for which slow recombination induces electron transfer phenomena described by Marcus theory. The spectacular long-lived radical pairs are attributed to the tight fit of the molecule in the channel, to the rate of aluminum and to the nature of the cation of the zeolite. These radical pairs are transient species in catalytic processes and photodegradation of hydrocarbon. They also take place in primordial reaction involved in photovoltaic effect.
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Matthieu Hureau. Séparation de charges de molécules linéaires insérées dans des zéolithes à canaux. Autre. Université des Sciences et Technologie de Lille - Lille I, 2007. Français. ⟨tel-00269880⟩

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