Introduction
Biodegradable polymers are growing mainly due to
ecological reasons [1–3]. Commercial starch based
blends are very useful for the management of
post-consumer waste and are used especially for
packaging industry [4–6].
Polymeric materials have been filled with several
inorganic synthetic and/or natural compounds in order
to increase several properties (especially mechanical
and impact properties) and decrease others (such as
gas permeability) [7–16].
In the case of crystalline polymers, mechanical and
physical properties are strongly dependent on the crystal
structure and morphology that are related with the
crystallization degree. Cyras et al. [4] have studied
the effect of natural fibres (sisal) on the crystallization
behaviour of MaterBi-Z (polycaprolactone/starch
blend). They have found that the Avrami exponent, n,
was close to 2 for the matrix and that this exponent
remained constant when sisal fibres were incorporated
up to 30 mass%. On the other hand, they demonstrated
that for a given crystallization temperature, the
induction time and the half-time of crystallization in-
creased with fibers incorporation (30 mass%). An
increase on the half-time of crystallization is related
with a decrease on the crystallization rate. Both
activation energies (for induction time and for the rate
constant) slightly increased when fibres were added.
In the case of nanocomposites, investigation of the
early stages of crystallization is of particular interest,
because of the possible role of clay platelets and tactoids
in crystal nucleation. It has been studied that clay
particulates greatly affects the crystallization behaviour
and morphology of polymer matrix. In several cases,
heterogeneous nucleation was observed [15, 17, 18].
Nanoparticles can either increase or decrease the
global crystallization rate of a semicrystalline polymer:
Fornes et al. [19] have shown that high clay
concentrations reduce the rate of crystallization in the
case of Nylon 6/MMT nanocomposites. Similar effects
have been observed for nanocomposites in other
matrices like PCL systems. Di Maio et al. [18] have
studied the case of PCL (polycaprolactone)/MMT.
They showed that the addition of 0.1% of nanoclay
resulted in a reduction of the crystallization half-time
to less than 1/2 of that of the pure matrix. The highest
crystallization rate was achieved with 0.4% of clay.
At higher nanoclay concentration, the crystallization
rate started to decrease. Furthermore, besides the
influence on nucleation, a retarding effect of the
silicate layers on the crystal growth of polymer
matrices has been found [19–21]. In the
crystallization of extruded PA-6 (polyamide-6)/MMT
nanocomposites, the overall crystallization rate
decreases with increasing silicate layer content at the
highest silicate layer contents, or even over the full
silicate layer content range [19].
Another important effect of clay incorporation is
the change on the crystallinity degree which is strongly
related with final mechanical properties.
Strawhecker et al. [22] have shown for PEO that the
enthalpy of melting (measured by DSC), showed no
strong effect of the silicate loading and/or the crystal-
1388–6150/$20.00 Akadémiai Kiadó, Budapest, Hungary
© 2008 Akadémiai Kiadó, Budapest Springer, Dordrecht, The Netherlands
Journal of Thermal Analysis and Calorimetry, Vol. 91 (2008) 3, 749–757
ISOTHERMAL CRYSTALLIZATION OF LAYERED
SILICATE/STARCH-POLYCAPROLACTONE BLEND NANOCOMPOSITES
C. J. Perez, A. Vázquez and V. A. Alvarez
*
Research Institute of Material Science and Technology (INTEMA), – National University of Mar del Plata (UNMdP)
Av. Juan B. Justo 4302, 7600 Mar del Plata, Argentina
The isothermal crystallization behavior of layered silicate/starch-polycaprolactone blend nanocomposites was studied by means of
differential scanning calorimetry (DSC) measurements. The theoretical melting point was higher for the matrix than for
nanocomposites. At low clay concentration, the induction time decreased and the overall crystallization rate increased acting as nu-
cleating agent whereas at higher concentrations became retardants. Classical Avrami equation was used to analyze the
crystallization kinetic of these materials. n values suggested that clay not only affected the crystallization rate but also influenced
the mechanism of crystals growth. An Arrhenius type equation was used for the rate constant (k). Models correctly reproduced the
experimental data.
Keywords: Avrami equation, biodegradable polymers, clays, crystallization, modeling, nanocomposites
* Author for correspondence: alvarezvera@fi.mdp.edu.ar