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Cooperativity Scaling and Free Volume in Plasticized Polylactide

Type
Articles dans des revues avec comité de lecture
Author
ARAUJO, Steven
301288 Institut national des sciences appliquées Rouen Normandie [INSA Rouen Normandie]
DELPOUVE, Nicolas
301288 Institut national des sciences appliquées Rouen Normandie [INSA Rouen Normandie]
DOMENEK, Sandra
148117 AgroParisTech
GUINAULT, Alain
86289 Laboratoire Procédés et Ingénierie en Mécanique et Matériaux [PIMM]
GOLOVCHAK, Roman
441141 Department of Physics & Astronomy [Clarksville]
SZATANIK, Roman
313012 University of Technology [Opole]
INGRAM, Adam
313012 University of Technology [Opole]
FAUCHARD, Cyrille
399153 CEREMA
DELBREILH, Laurent
301288 Institut national des sciences appliquées Rouen Normandie [INSA Rouen Normandie]
DARGENT, Eric
301288 Institut national des sciences appliquées Rouen Normandie [INSA Rouen Normandie]

URI
http://hdl.handle.net/10985/19449
DOI
10.1021/acs.macromol.9b00464
Date
2019
Journal
Macromolecules

Abstract

The experimental evidence of the increase of activation energy associated with the super Arrhenius behavior governing amorphous polylactide by free volume variations has been obtained through a combination of calorimetric, dielectric, and positron annihilation lifetime measurements. The amount of free volume in polylactide was controlled by the amount of acetyltributylcitrate plasticizer in the composition. Plasticization is shown to decrease both the fragility index and the scale of cooperative motions at the glass transition. The calculations of volume and energetic components of kinetic fragility reveal that the fragility drop is governed by the change in the size of cooperative rearranging region. As a result, direct correlation has been established between cooperativity and activation energy for the entire plasticized polylactide series. It is also shown that cooperativity variations with both temperature and plasticizer content can be simplified as a master curve with free volume.

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