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Heat seal characteristic of environmental friendly films from thermoplastic rice

starch filled poly(lactic acid)

Article · January 2013

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Supaphorn Thumsorn Sommai Pivsa-Art

Yamagata University Rajamangala University of Technology Thanyaburi
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 HEAT SEAL CHARACTERISTIC OF ENVIRONMENTAL FRIENDLY FILMS
FROM THERMOPLASTIC RICE STARCH FILLED POLY(LACTIC ACID)
Supaphorn Thumsorn and Sommai Pivsa-Art, Rajamangala University of Technology Thanyaburi,
Pathumthani, Thailand
Ken Miyata, Yamagata University, Yamagata, Japan
Kazushi Yamada and Hiroyuki Hamada, Kyoto Institute of Techmology, Kyoto, Japan
Abstract
An environmental friendly biodegradable polymer
film was prepared from poly(lactic acid)/thermoplastic
starch (PLA/TPS) blend by cast film process at 0, 5 and
10 wt% of TPS. The PLA/TPS blend films were heat
sealed by a heat seal tester at a heat bar temperature of 90
and 100 C. The heat seal time was varied from 0.5 to 2.0
s with a constant seal pressure of 0.2 MPa. The effect of
heat seal conditions on heat seal properties of PLA/TPS
films was investigated. Heat sealed strength was carried
out by peel testing. Differential scanning calorimetry was
used to analyze thermal properties and crystallinity of the
heat sealed PLA/TPS films. From the results, heat sealed
strength of PLA/TPS blend films decreased when
increasing the heat sealed times. PLA films was peelable
at the heat sealed temperature of 90 C. PLA/TPS heat
sealed films exhibited greater crystallinity than the PLA
heat sealed film.
Introduction
The heat sealability of a material is a major property
to maintain the integrity of a package, especially in
medical, food packaging, pharmaceutical applications,
and so on. To obtain a proper heat seal is of paramount
importance in packaging because heat seal failure is a
more frequent cause of product deterioration than the
failure of the package itself. Selecting the right material
that will perform under the right conditions requires
careful consideration of the functional requirements of the
package and the method of packaging.
In the present day, biodegradable plastics have been
introduced for packaging industries due to the emphasis
on the environmental consideration. The biodegradability
of biodegradable plastics would overcome for less
garbage, reducing energy for incineration and lack of land
fill space. The various kinds of biodegradable plastics
packaging are available. Nevertheless, the drawbacks of
biodegradable plastics are still high cost and low thermal
resistance. Therefore, biodegradable fillers such as starch
and clay are adding for obtaining low cost plastic film
packaging and enhancing their thermal resistance [1-2].
Moreover, heat seal technology is an essential technique
for intermediate packaging industries.
Miyata et al [4-5] studied the effect of molecular
weight and cast film conditions on heat seal properties of
high density polyethylene (HDPE) film. They found that
the heat seald conditions were important factors to affect
molecular structures, which was also an important for heat
seal properties. Heat seal strength changed depending on
cast film conditions. In low chilled roll speed heat seal
strength was low. The failure mode was peeling. In high
chilled roll speed heat seal strength was high. The failure
mode was changed to tearing. Tetsuya et al [6] focused on
the effect of heat sealed temperature on properties of
polypropylene (PP) films. Their researchs gave
information on the relation between heat seal strength,
crystallinity and molecular orientation of PP films. Yuan
et al [7] investigated heat sealability of laminated films
with linear lowdensity PE (LLDPE) and low density PE
(LDPE) as sealants. This research revealed that heat seal
strength responsed to laminated film temperature, time
and pressure. However, there are very few researches on
the sealability of biodegradable film materials. Therefore,
it is important to investigate the heat seal characteristic of
biodegradable plastics and mechanical performance of
these materials upon heat sealing.
In this study, the biodegradable plastic films of PLA
filled with rice starch were prepared. The heat sealed of
the biodegradable plastic films was performed by thermal
heat sealed method. In order to evaluate the effects of heat
sealed parameters on the quality of the seal, heat-sealing
was performed at several temperatures and the strength of
heat sealed part was evaluated. This research will perform
the heat seal characteristic of rice starch filled
biodegradable plastic films for utilization in packaging
applications
Experimental
Poly(lactic acid) (Grade 2002D) was supplier by
NatureWorks LLC, USA. The melt fow rate was 5 g/10
min. Thermoplastic starch (TPS) was prepared from
mixing rice starch with 30 wt% glycerol in a twin screw
extruder (Lab Tech Engineering, Thailand). The bareel
temperature was set at 100-120 C with a screw apeed of
80 rpm. After pelletized, TPS was dried at 60 C for 12
hours. PLA and TPS films were fabricated by a twin
ANTEC® 2013 / 1331
screw extruder (KZW-30; Technovel Co., Ltd., Japan) films at sealing temperature of 100 C decreased with
equipped with T die. The ratio of length and diameter, increasing heat sealed times. At this heat sealed
L/D, of the screw was 45. The extruder barrel temperature temperature, all films were pulled out such a suddenly
was set at 150-190 ºC. The T-die temperature was set at tearing. It can be note that the temperature higher than 100
190 ºC. The thickness of extruded film was controlled to C was not suitable for peelable PLA and PLA/TPS films.
around 50 μm by chilled roll and screw rotating speed.
The PLA/TPS films were done with varied contents of Table 1. Heat seal strength of PLA and PLA/TPS films.
TPS from 5 and 10 wt%. The films were then referred as
PLA/TPS-5 and PLA/TPS-10 for the films of adding TPS Heat sealed strength
5 wt% and 10 wt%, respectively. PLA films were also Temperature (N/15 mm)
Samples
prepared as controlled. (C)
0.5 s 1.0 s 2.0 s
Extruded PLA/TPS films were heat sealed by using a PLA 22.33 22.16 26.31
heat seal tester (TP-701-B; Tester Sangyo Co., Ltd.). Two 90 PLA/TPS-5 23.38 20.65 18.72
pieces of the film were thermally sealed near their melting PLA/TPS-10 22.37 20.20 11.25
temperature. The heat bar temperature was varied at 90 ºC
and 100 ºC. The seal pressure was kept constantly at 0.2 PLA 26.51 19.40 18.23
MPa. The heat seal time was varied from 0.2 to 2.0 100 PLA/TPS-5 20.98 17.91 9.22
seconds. PLA/TPS heat sealed films were cut to 100 mm PLA/TPS-10 18.25 7.20 5.87
long and 15 mm wide for peel testing.

Peel testing of PLA/TPS heat sealed films specimens 30

Heat sealed 90 C
was carried out by universal tensile testing machine Heat seal strenght (N/15 mm)
(Hounsfield) with the extension rate of 300 mm/min. 25

Thermal properties and crystallinity of the films 20

before and after heat sealed were analyzed by differential
scanning calorimetry (NETZSCH, DSC 200 F3) at 30- 15
200 C at heating and cooling rate of 10 C/min.
10
Results and Discussion
5
Heat seal strength of PLA and PLA/TPS films PLA PLA/TPS-5 PLA/TPS-10
0
The effect of heat sealed temperature and time on 0.0 0.5 1.0 1.5 2.0 2.5
heat seal strength of PLA and PLA/TPS films is tabulated Heat seal time (s)
in Table 1 and depicted in Figures 1 and 2. Table 1
Figure 1. Heat seal strength of the films at heat sealed
summarizes the heat seal strength of PLA and PLA/TPS
temperature 90 C.
films. Healt seal strength of the films exhibited
declination when increasing heat sealed temperatures and 30
times. Heat sealed 100 C
Heat seal strenght (N/15 mm)

25
Figure 1 presents the heat seal strength of films at
heat sealed temperature of 90 C. The heat seal strength
20
was approximately 22 N/15 mm. However, heat seal
strength of the PLA/TPS films decreased with increasing
15
heat sealed time. The films were torn and separated
without peeling at the heat sealed part. The failure mode
of these films was tearing failure [4]. The results indicated 10
that this heat sealed temperature was too high for
fabricating PLA/TPS heat sealed films. On the other hand, 5
the heat sealed strength of the PLA films increased when PLA PLA/TPS-5 PLA/TPS-10
heat sealed time increased. The PLA films were well 0
adhered at this temperature and peelable at the 0.0 0.5 1.0 1.5 2.0 2.5
temperature lower than 2.0 s. The failure mechanism of Heat seal time (s)
PLA heat sealed films was peeling and adhesive failure Figure 2. Heat seal strength of the films at heat sealed
[4]. On the contrary, the heat sealed strength of the all temperature 100 C.

ANTEC® 2013 / 1332

Thermal properties of PLA and PLA/TPS films
Thermal properties and crystallization of PLA and
PLA/TPS films before and after heat sealed were carried
out by differential scanning calorimetry (DSC). The
results are illustrated in Figures 3-7. Figure 3 shows
thermograms of neat PLA and PLA/TPS films before heat
sealing. These thermograms exhibited endothermic and
exothermic peaks during the melting. The slope at around
60 C indicated glass transition temperature of PLA
followed by the exothermic peak of precrystallization
(cold crystallization) of PLA at about 120 C. It can be
seen that the addition of TPS in the PLA improved PLA
crystallization by presented the lower in cold
crystallization temperature as compared to the PLA film
[8].
2.0
PLA PLA/TPS-5
1.6
Heat flow endo up (W/g)
temperature 90 C for 0.5-2.0 s. The thermograms
exhibited the faster of cold crystallization in the films that
heat sealed for 0.5 s, which this point the films could be
obtain higher crystallinity than the others. Therefore, the
increment in heat sealed time in PLA/TPS films would not
yield in an enhancement of heat seal strength as can be
seen in the heat sealed strength results.
Figure 6 exhibits the effect of heat sealed temperature
on thermal properties and crytallization of PLA and
PLA/TPS films. The results showed the thermograms
comparison between PLA and PLA/TPS films at heat
sealed temperature of 90 and 100 C. From the results,
higher heat sealed temperature affected on the shift of the
cold crystallization temperature of PLA in the films. The
lower heat sealed temperature of 90 C was better in
crystallization.
2.0
PLA/TPS-10 Heat sealed 90 C 1.0 s

1.6 PLA PLA/TPS-5 PLA/TPS-10

1.2 Heat flow endo up (W/g)

1.2
0.8
0.8
0.4
0.4
0.0
30 60 90 120 150 180 0.0
Temperature (C) 30 60 90 120 150 180
Temperature (C)
Figure 3. DSC thermograms of the films before heat
Figure 4. DSC thermograms of heat sealed films at heat
sealed.
sealed temperature 90 C for 1.0 s.
The endothermic peaks around 154 C indicated melting
2.0
temperature of PLA. TPS influenced on PLA PLA/TPS-5
crystallization by presented a small peak in the melting
endothermic peak, which resulting from the melting of 1.6 0.5 s 1.0 s 2.0 s
Heat flow endo up (W/g)

difference PLA crystal sizes in these PLA/TPS films [9].

1.2
Figure 4 depicts DSC thermograms of the heat sealed
films at 90 C for 1.0 s. From the results, glass transition
temperature and melting temperature of PLA in the films 0.8
were unchanged after heat sealing. However, the cold
crystallization temperature of PLA heat sealed films was
0.4
lower than in the PLA/TPS films. Therefore, crystallinity
of PLA film was higher than the PLA/TPS one. It can be
seen that the heat seal strength of the PLA film was also 0.0
higher than that of PLA/TPS films. Therefore, 30 60 90 120 150 180
crystallinity influenced on enhanced the heat seal stregth. Temperature (C)
Figure 5. DSC thermograms of heat sealed PLA/TPS-5
The effect of heat sealed time on thermal properties films films at heat sealed temperature 90 C with varied
of the films was presented in Figure 5. Figure 5 shows the heat sealed times.
thermograms of PLA/TPS-5 films at heat sealed

ANTEC® 2013 / 1333

 2.0 2.5
PLA-90 C PLA-100 C Heat sealed 100 C
PLA/TPS-10-90 C PLA/TPS-10-100 C

Endothermic enthalpy (J/g)

1.6 2.0
Heat flow endo up (W/g)

1.2 1.5

0.8 1.0

0.4 0.5
PLA PLA/TPS-5 PLA/TPS-10
0.0 0.0
30 60 90 120 150 180 0.0 0.5 1.0 1.5 2.0
Temperature (C) Heat seal time (s)
Figure 6. DSC thermograms of heat sealed films at heat Figure 8. Effect of heat sealed time on endothermi
sealed temperature 90 C and 100 C for 2.0 s. enthalpy of heat sealed films at 100 C.
Figures 7 and 8 illustrate endothermic enthalpies of PLA heat selaed films, which exhibited peeling
the heat sealed films at heat sealed temperature of 90 and characteristic in failure mode. On the other hand, these
100 C, respectively. The enthalpy of PLA heat sealed heat sealed temperatures and times were not suitable for
film exhibited higer than the PLA/TPS films. It indicated improved the heat seal strength of PLA/TPS films, which
that the crystallinity of PLA films was better than the the PLA/TPS heat sealed film presented tearing in failure
others. The DSC results could be considered that the mode. The improvement of heat seal strength and
crystallinity of the films depended on heat sealed peelability of PLA/TPS films might be obtain when using
temperature, time and the composition of the films. It is the heat sealed temperature lower than 90 C.
intersting to note that the heat sealed films with higher
crystallinity would be resulting in better heat seal strength.
Acknowledgment
2.5 The authors greatfully acknowledge Thailand
Heat sealed 90 C
Research Fund (TRF) for supporting a research grant for
Endothermic enthalpy (J/g)

2.0 new scholar (MRG2555) contact no. MRG5580020.

1.5
References
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The heat sealed temperature of 90 C provided peelable of

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