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Organisation multi-échelle de matériaux polymères contrôlée par la chimie aux interfaces

Abstract : Materials properties very often derive from their nano or micro-scale organization. In this thesis, we evidence that controlling the chemistry at the interfaces allows obtaining spontaneously very regular organizations in various polymer materials.In the first part, supramolecular chemistry has been used to control the organization in the bulk of polymer grafted at one or both extremities by thymine (Thy) or 2,6-diamino-1,3,5-triazine (DAT), two self-complementary supramolecular units interacting via hydrogen bonds. Whatever the polymer nature (PE, PDMS, PPG), materials present very regular nanoscale long-range ordered lamellar organizations if the end group crystallize (Thy) and/or the chain crystallize (PE). Respective contributions to these organizations of phase segregation, crystallization, supramolecular interactions and secondary interactions have been determined. It was shown that the confinement of chains in lamellae prevent the formation of high molecular weight chains, resulting in poor mechanical properties. However, Thy/DAT interactions allow creating supramolecular block copolymers by mixing incompatible chains functionalized with these units.In the second part, we have studied the spontaneous formation of patterns at the film surface of acrylate film during their photopolymerization under air. This phenomenon occurs if there is a balance at the film surface between the polymerization and the oxygen inhibition rates. Very regular microscale patterns (hexagons, lamellae, peanuts) have been generated by controlling some experimental parameters (UV intensity, initiator concentration) for a wide range of film thicknesses (6 µm – 2 mm). Self-patterning gives interesting optical properties to the films (haze, clarity) which can be modulated by adjusting the patterns wavelength and amplitude.
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Jérémie Lacombe. Organisation multi-échelle de matériaux polymères contrôlée par la chimie aux interfaces. Matériaux. Université Paris sciences et lettres, 2017. Français. ⟨NNT : 2017PSLET012⟩. ⟨tel-02918064⟩

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