Studies on Nylon-6/EVOH/Clay Ternary Composites
N. Artzi, B.B. Khatua, M. Narkis
Department of Chemical Engineering, Technion—Israel Institute of Technology, Haifa 32000, Israel
A. Siegmann
Department of Materials Engineering, Technion—Israel Institute of Technology, Haifa 32000, Israel
Nylon-6 (Ny-6)/EVOH blends are interesting host mul-
tiphase systems for incorporation of low clay contents.
The Ny-6/EVOH blend is a unique system, which tends to
chemically react during melt-mixing, affecting thermal,
morphological and mechanical properties of the ternary
systems containing clay. The addition of clay seems to
interrupt the chemical reaction between the host poly-
mers at certain compositions, leading to lower blending
torque levels when clay is added. A competition between
Ny-6 and EVOH regarding the intercalation process
takes place. Ny-6 seems to lead to exfoliated structure,
whereas EVOH forms intercalated structure, as revealed
from XRD and TEM analyses, owing to thermodynamic
considerations and preferential localization of the clay in
Ny-6. Hence, the ternary systems have combined inter-
calated and delaminated morphology or complete exfo-
liated morphology depending on blend composition and
clay content. Selective extraction experiments (gel con-
tent) indicate the formation of chemical reaction be-
tween the Ny-6 and EVOH, and give an indirect indica-
tion of the polymer content residing in the galleries. The
thermal properties of the polymers were found to be
affected by the occurrence of chemical reaction, the
level of intercalation and exfoliation and plasticizing ef-
fect of the low molecular weight onium ions treating the
clay. Of special interest is the increased storage modu-
lus attained upon the addition of only 1.5 wt% clay.
POLYM. COMPOS., 27:15–23, 2006. © 2005 Society of Plastics
Engineers
INTRODUCTION
Nanocomposite materials consisting of organic polymers
and inorganic clay have recently evoked intense research
interests owing to their unique characteristics [1]. From the
point of view of obtaining improved physical/mechanical
properties of nanocomposites, exfoliation is preferred to
intercalation. In general, intercalation is observed when the
polymer matrix and the clay have intermediate interaction
levels, while exfoliation is observed when the polymer and
the clay have strong attractive interactions. Hence, as in the
preparation of immiscible polymer blends, compatibility
between the polymer and clay is desired [2].
Multiphase polymer blends have been of great impor-
tance in the development of new synthetic materials. How-
ever, polymer blends usually result in heterogeneous, two,
or multiphase materials exhibiting poor properties. Al-
though the limited components miscibility is sometimes
used to improve specific properties, generally immiscibility
of the polymers hinders utilization of their blends. The
general challenge of polymer blending is to overcome the
low entropy of mixing and unfavorable enthalpy of mixing
typical of most high molecular weight polymers. The
achievement of compatibilization, whether by addition of a
third component (i.e., compatibilizer) or by in situ chemical
reactions between the blend’s components (reactive blend-
ing) has played an important role in the development of
polymer blends [3]. Ethylene vinyl alcohol (EVOH) copol-
ymers appear to have the potential of forming compatible or
even miscible blends in the amorphous state with a variety
of polymers containing functional groups such as esters,
methacrylates, acetoxys, ethers, and the like [4]. The tech-
nological incentive toward nylon/EVOH blends is in pack-
aging applications. Polyamides are engineering semicrystal-
line thermoplastics having low permeability for CO
2
, while
EVOH copolymers are semicrystalline materials showing
excellent oxygen barrier properties in their dry state [5].
Nanocomposites based on organoclays and homopoly-
mers have been extensively investigated; however, nano-
composites based on organoclays dispersed in immiscible
polymer blends are relatively rare although novel materials,
which combine the properties of polymer blends and nano-
metric clays, can be visualized. It is expected that such
materials will differ in the level of clay dispersion (e.g., the
extent of exfoliation/intercalation of layered silicates) and
the blend phase morphology (e.g., the average size of phase-
separated domains) compared with single polymer/clay
Correspondence to: M. Narkis; e-mail: narkis@tx.technion.ac.il
Contract grant sponsor: Levi Eshkol scholarship of the Israel Ministry of
Science.
DOI 10.1002/pc.20157
Published online in Wiley InterScience (www.interscience.wiley.
com).
© 2005 Society of Plastics Engineers
POLYMER COMPOSITES—2006