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Reducing the Gap between the Activation Energy Measured in the Liquid and the Glassy States by Adding a Plasticizer to Polylactide

Article dans une revue avec comité de lecture
Author
ARAUJO, Steven
520133 Centre d'Etudes et d'Expertise sur les Risques, l'Environnement, la Mobilité et l'Aménagement - Direction Normandie-Centre [Cerema Direction Normandie-Centre]
970 Groupe de physique des matériaux [GPM]
DELPOUVE, Nicolas
970 Groupe de physique des matériaux [GPM]
300318 Université de Rouen Normandie [UNIROUEN]
441569 Centre National de la Recherche Scientifique [CNRS]
455934 Normandie Université [NU]
DHÔTEL, Alexandre
970 Groupe de physique des matériaux [GPM]
DOMENEK, Sandra
419361 Université Paris-Saclay
549820 Ingénierie, Procédés, Aliments [GENIAL]
GUINAULT, Alain
86289 Laboratoire Procédés et Ingénierie en Mécanique et Matériaux [PIMM]
DELBREILH, Laurent
970 Groupe de physique des matériaux [GPM]
DARGENT, Eric
970 Groupe de physique des matériaux [GPM]
115914 Human Computer Technology Laboratory [HCTLab]

URI
http://hdl.handle.net/10985/15415
DOI
10.1021/acsomega.8b02474
Date
2018
Journal
ACS Omega

Abstract

The kinetic fragility of a glass-forming liquid is an important parameter to describe its molecular mobility. In most polymers, the kinetic fragility index obtained from the glassy state by thermally stimulated depolarization current is lower than the one determined in the liquid-like state by dielectric relaxation spectroscopy, as shown in this work for neat polylactide (PLA). When PLA is plasticized to different extents, the fragility calculated in the liquid-like state progressively decreases, until approaching the value of fragility calculated from the glass, which on the other hand remains constant with plasticization. Using the cooperative rearranging region (CRR) concept, it is shown that the decrease of the fragility in the liquid-like state is concomitant with a decrease of the cooperativity length. By splitting the fragility calculated in the liquid, in two contributions: volume and energetic, respectively, dependent and independent on cooperativity, we observed that the slope of the fragility plot in the glass is equivalent to the energetic contribution of the fragility in the liquid. It is then deduced that the difference between the slopes of the relaxation time dependence calculated in both glass and liquid is an indicator of the cooperative character of the segmental relaxation when transiting from liquid to glass. As the main structural consequence of plasticization lies in the decrease of interchain weak bonds, it is assumed that these bonds drive the size of the CRR. In contrast, the dynamics in the glass are independent on plasticization structural effects.

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