Abstract:
Some novel biodegradable polymer composites were synthesized, using polyolefin as a
matrix with various natural polymers including chitosan, starch and carboxymethyl
cellulose as biodegradable additives. The compatibility of the components was enhanced
with different silane coupling agents. The materials were heat mixed in brabender plasti-
corder mixer using roller rotor. During mixing, different temperatures were used to mix
and decompose the initiator to start the grafting of silane and crosslinking of the
polymer. The blended materials were hot pressed into sheets. The hydrolysis and the
condensation reactions of silane were carried out in hot water at 95°C for 20 hours. After
crosslinking reactions, the prepared sheets were dried in vacuum oven for 16 hours
before characterization.
The structural analysis of the non-crosslinked and crosslinked composites was carried
out using Fourier Transform Infrared (FTIR) and Scanning Electron Microscope (SEM)
techniques. The crosslinking reaction was confirmed by FTIR spectra, which revealed
the important absorption peaks of siloxane (Si-O-Si) and Si-O-C bonds. SEM images
also revealed that crosslinking has improved the dispersion and interaction between
polymer and the additives. The degree of crosslinking as determined by gel content
analysis was found to be directly proportional to the amount of chitosan in
HDPE/chitosan composite. In LLDPE/starch/sepiolite composite, it decreased with high
sepiolite loading. Thermogravimetric analysis showed higher thermal stability of the
crosslinked composites. Differential scanning calorimetry showed decreasing trend of
percentage crystallinity with increasing amount of additive. This behavior is associated
to the network structure and the disorder of close packing of polyethylene chains.
Rheological studies of crosslinked composites showed linear viscoelastic behavior with
high complex viscosities (*) and dynamic shear storage moduli (G`) reflecting a strong
interaction between matrix-filler interphase and the elastic nature of the crosslinked
samples. High tensile strength (TS) and reduced elongation at break (Eb) values were
observed in all the crosslinked samples of HDPE/chitosan and HDPE/carboxymethyl
cellulose composites. However, the TS and Eb values of non-crosslinked and crosslinked
formulations for LLDPE/starch/sepiolite composite showed decreasing trends with high
starch and sepiolite loading. Creep experiments indicated a small deformation in
crosslinked composites, which showed that silane effectively coupled the immiscible
components.