Polymer Testing 46 (2015) 116e121

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Polymer Testing
journal homepage: www.elsevier.com/locate/polytest

Material behaviour

Investigating the effect of accelerated weathering on the mechanical

and physical properties of high content plastic solid waste (PSW)
blends with virgin linear low density polyethylene (LLDPE)
S.M. Al-Salem a, *, G. Abraham b, O.A. Al-Qabandi c, A.M. Dashti b
a
Environment & Life Sciences Research Centre, Kuwait Institute for Scientific Research, P.O. Box: 24885, Safat 13109, Kuwait
b
Petroleum Research Centre, Kuwait Institute for Scientific Research, P.O. Box: 24885, Safat 13109, Kuwait
c
R&D Department, EQUATE Petrochemical Company, P.O. Box: 91717, Ahmadi 61008, Kuwait

a r t i c l e i n f o a b s t r a c t

Article history: In developing countries, plastic solid waste (PSW) poses a serious threat due to the increase in the
Received 23 June 2015 dependency on landfilling as well as other environmental issues. Hence, valorising the accumulated
Accepted 27 July 2015 waste is essential to promoting more environmentally friendly practices. In this work, the mechanical
Available online 29 July 2015
and physical properties of virgin linear low density (LLDPE) and LLDPE blends with PSW are reported.
The formulations studied contained the following virgin to waste ratios (wt.%/wt.%): 100/0, 75/25, 50/50,
Keywords:
25/75 and 10/90. The effect of photo-degradation on the studied specimens was investigated using
LLDPE
accelerated weathering tests in a UV chamber. Young's modulus showed an increase with exposure
Weathering
Degradation
duration due to change in the samples' crystallinity. The loss of mechanical integrity (i.e. stress and strain
Haze at rupture) of the samples studied was related to the photo-degradation mechanisms, namely cross-
Light transmission linking and photo-oxidation. Haze and light transmission measured indicated that there was a loss of
Waste the amorphous regions in the samples studied after about 200 h of continuous exposure. The total
Polyolefins change in colour (DE) was estimated but did not show a clear trend, indicating a clear dependency on
wash mechanism and continuous loss of polymer colour and degradation.
© 2015 Elsevier Ltd. All rights reserved.

1. Introduction market is dominated by polyolefin polymers. These include linear

In developing countries, plastic solid waste (PSW) constitutes a
considerable proportion of municipal waste (MSW). Furthermore,
in the State of Kuwait, it makes up over 13% of MSW with an esti-
mated 200 ktonnes in the year 2014 [1e3]. This has resulted in a
concerted effort to reduce the landfill space required and to pro-
mote environmental solutions to disposing of this ever growing
fraction of waste. Mechanical treatment of polymer waste presents
a number of advantages including the creation of job opportunities,
the reduction of the carbon footprint of polymer resin production
and the reduction of the processing costs of plastic converters.
The study of polymer degradation helps to develop products
with outdoor applications. It determines the service life of plastic
compounds and gives a detailed analysis of the degradation
behaviour that a polymer blend exhibits. The commodity plastics
* Corresponding author.
E-mail address: ssalem@kisr.edu.kw (S.M. Al-Salem).
low density polyethylene (LLDPE) in addition to high density
polyethylene (HDPE), low density polyethylene (LDPE) and poly-
propylene (PP). These polyolefins are used extensively in packaging
and outdoor applications, which leads to their accumulation in
MSW. LLDPE possesses mechanical and optical properties that are
superior to all other polyolefins which has led to its use in a number
of areas. Production of polyolefins, namely LLDPE, has increased
worldwide. In the Middle East, recent estimates show a production
increase in capacity of over five times that of the year 2000 [4].
Weathering of polymers is an established technique to deter-
mine the extent of degradation a polymer suffers. It is essential to
evaluate the properties of samples intended to be used in the future
for various outdoor applications under different exposure condi-
tions. In literature, there are few articles that show the weathering
effect on virgin/waste polymer blends [5,6]. The history of the PSW
used in the blend is essential in developing these blends. Weath-
ering is typically studied on virgin polymers with and without
additives (e.g. antioxidants, light transformers, stabilisers, etc.) to
determine the durability and extent of degradation of the

http://dx.doi.org/10.1016/j.polymertesting.2015.07.008
0142-9418/© 2015 Elsevier Ltd. All rights reserved.
 S.M. Al-Salem et al. / Polymer Testing 46 (2015) 116e121
polymeric article [7e9]. The mechanical properties of HDPE com-
pounded with fillers were studied by Lundin et al. [10] after
accelerated weathering. The Young's modulus was reported to have
increased during the first half of the weathering period by about
70%. Zhao et al. [11] reported the effect of exposure to accelerated
weathering on LLDPE/LDPE films, concluding that a correlation
might be validated with natural exposure. Mourad [12] reported
the effect of accelerated weathering on blends of polyethylene (PE)
and polypropylene (PP). It was concluded that PE was the polymer
which governed the properties of the blend, causing a decrease in
yield strength as its content increased.
In this work, the degradation effect on virgin LLDPE and virgin
LLDPE blends with PSW originating from plastic waste films is
studied. The mechanical properties (i.e. Young's modulus, stress,
strain and force at rupture) and physical properties (i.e. haze, light
transmission and total change in colour) of the studied specimens
are reported. To the best of our knowledge, no study on the
degradation of different formulations of virgin and waste plastic
films using accelerated weathering on blends with no additives has
been reported previously in literature. The work in this paper could
lead to the development of products for outdoor applications and
reduce the impact of PSW on the environment. In addition, it gives a
detailed analysis of polymeric blend degradation originating from
mechanically compounding virgin and waste polymers.
2. Experimental
2.1. Materials and film sample preparation
Plastic waste (200 kg) secured from the National Waste Man-
agement Company (Kuwait) in the form of plastic films from
various sources collected in the state of Kuwait was used in this
study. The waste material constituted the following percentages of
the polymers (wt.%): LLDPE (46%), LDPE (51%), HDPE (1%) and PP
(2%). The waste films were milled to 3
3 mm flakes using a Tec-
nova cutting mill and pelletized to 3
3 mm pellets using a Tec-
nova industrial single screw extruder (L/D ¼ 30) at 40 bar pressure
and 70 RPM. The cooling water temperature was maintained be-
tween 16 and 17  C. Linear low density polyethylene (LLDPE) was
graciously supplied by the EQUATE Petrochemical Company
(Kuwait) and used in this work as white translucent pellets with a
density of 0.918 g/cm3 and a melt flow index (MFI) of 2 g/10 min.
For the purpose of confidentiality, the company did not provide
details of the additives in this commercial grade.
Dry blends (i.e. with no additives at the blending stage) of both
virgin and waste polymers were weighed, extruded and blown
using a single screw extruder (Tecnova, L/D ¼ 30, 45 bar and 85
RPM) and a film blowing machine (Kung Hsing monolayer) with a
water cooling temperature maintained between 16 and 17  C. Die
head temperature of the extruder was maintained at 175  C, with
the six zones maintained at 175e185  C. The virgin LLDPE to waste
ratios (in weight) considered in this study were 100/0, 75/25, 50/50,
75/25 and 10/90. The extruded sheets of 100 mm thickness were cut
using a standard cutting die (Ray Ran UK cutting press - model RR/
PCP) to produce 20
1 cm films for further characterisation. The
samples appeared consistent with no visual fractures or crazing and
were comparable to each other by touch. All samples were stored in
laboratory conditions at 23  C/50% relative humidity and in the
dark between sample formulation and testing.
2.2. Accelerated weathering
Films of the different formulations were exposed to accelerated
weathering in accordance with ASTM 4329 [13]. Samples were
mounted on the racks facing the UV lamps with no empty spaces in
117
the panels in order to maintain repeatable test conditions. Cycle A
procedure was used for general applications, i.e. 8 h of UV exposure
at 60  C followed by 4 h of condensation at 50  C. At the end of each
continuous weathering test, the chamber was cooled to room
temperature and trays were set to rest on a flat surface for a mini-
mum of 24 h. Samples were laid to rest for a minimum of 72 h before
characterisation following the methodology of Johnson et al. [14].
2.3. Mechanical properties
The evaluation of mechanical properties was conducted at room
temperature to determine the impact of weathering on the film
samples following ASTM D882 [15]. Experiments were conducted
using a Testometric (UK) universal testing machine-model
DBBMTCL-250 kg (M250-2.5 kN load cell) with a 500 mm/min
speed. The measured properties include: Young's modulus (MPa),
the stress at rupture (MPa), the strain at break (%) and the force at
break (N). The measurement values obtained came from the
average of 5 replicate specimens stored directly from the machine's
software.
2.4. Haze and transmission measurements
A Diffusion System MF709 (spherical) haze meter (model BS
2782) was used to measure the haze and transmission at the
midpoint of the studied samples, in accordance with ASTM D1003
[16]. Replicates of the tested specimens were tested for haze (%) and
light transmission (%) and the average of the readings is reported.
2.5. Colour parameters
Standard colour parameters for light/dark (L*s ), red/green (a*s )
and yellow/blue (b*s ) were measured using a Nippon Denshoku
model NF333 colorimeter according to ASTM D2244 [17]. Parame-
ters measured were then used to calculate the total change in
colour between control samples and each weathered formulation
thus [17,18]:
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
DE ¼ ðDLÞ2 þ ðDaÞ2 þ ðDbÞ2 (1)
where DL, Da and Db are the values of the difference between the
control specimen measurements (control samples with no expo-
sure to weathering) and those of each tested batch. The average
readings of the replicates for each formulation were measured and
are reported in this work.
3. Results and discussion
3.1. Young's modulus
Fig. 1 shows the Young's modulus measured for the different
blends at different exposure times. Overall, an increase was seen
with respect to the duration of weathering. Virgin LLDPE showed an
increase of approximately 30% as compared with control speci-
mens, i.e. with no exposure. The increase was incremental, reaching
its maximum value (z109 MPa) at the threshold limit (360 h of
continuous exposure). The Young's modulus is dependent on the
crystallinity of the polymer [10,12,19]. UV irradiation leads to
photo-degradation of the polymer via a well-established mecha-
nism which has been reported previously by a number of authors
[8,10,11,19]. The degradation of PE is initiated with chain scission,
then branching, cross-linking and terminates with a double bond
formation. One of the irreversible alterations of photo-degradation
is the loss of amorphous regions due to cross-linking, which can be
118
160
140
120
Young's Modulus (MPa)
100
80
60
40
20
0 showed a slight increase of stress at rupture for control specimens
0 50 100 150 200 250
Exposure Duration (Hours)
Fig. 1. Young's modulus (MPa) as a function of accelerated weathering duration
(hours).
attributed to the change in the Young's modulus of virgin resin
samples (Fig. 1).
The 75/25 (wt.%/wt.%) blend showed a similar threshold limit,
withstanding 360 h of continuous exposure to accelerated weath-
ering. The 50/50, 25/75 and 10/90 (wt.%/wt.%) of virgin/waste for-
mulations had just over 260 h of threshold limit to continuous
accelerated weathering, which is less by about 100 h (about 4 days)
compared to the others. The addition of the plastic waste increased
the modulus by an average of 30 MPa at different exposure dura-
tions. The waste material used contains different types of polymers
which undergo different heat cycles and thermal processing con-
ditions. The PE fraction in the waste, which constituted the highest
proportion, underwent three different heat cycles. Initially, the
polymer was converted to the plastic product. Consecutively, it was
pelletized and re-processed again to formulate the studied blends
in this work. The PP in the waste films used also underwent similar
thermal processing stages. Photo-oxidative degradation of poly-
mers due to oxygen diffusion in the polymer's matrix occurs at
different thermal processing stages which causes hydroperoxide
formation [8]. PE and PP both suffer from this phenomenon to
different degrees, with PP being more susceptible due to its
possession of high frequency tertiary atoms. This was evident in the
trends observed experimentally for the modulus, since a higher
waste content led to a higher modulus which can be attributed to
higher crystallinity, resulting in the material being more brittle. The
90/10 (wt.%/wt.%) blend showed recovery of the modulus in the last
third of the weathering exposure time. This could be attributed to
the waste content acting as a pseudo polymer that has deteriorated
more than the Virgin LLDPE, which leads to a higher modulus.
The films of 90/10 (wt.%/wt.%) did not withstand longer dura-
tions of weathering for the mechanical properties to be measured
at durations stretching over 264 h of weathering. Previous results of
natural weathering in Kuwait suggest that 24 h by ASTM standards
of artificial weathering can be correlated to 430 h of natural
exposure [18]. Correlating artificial and natural weathering is
polymer type dependent and cannot be applied except when
verified against actual natural exposure durations of similar tested
specimens [20]. However, it can give an indication to the extent that
the polymeric article withstands natural exposure, which in this
study is estimated to be about 9 months. On visual examination, the
addition of waste to virgin polymer in the blends studied resulted
in more discolouration (yellowness in colour) to the samples. This
could be a direct result of the loss of the transparency of the virgin
polymer material and the increase in the additive content in the
blends, originating from the waste material. Plastic films converted
in Kuwait will typically contain stabilisers, pigments and
S.M. Al-Salem et al. / Polymer Testing 46 (2015) 116e121
antioxidants from the various resins used which, after extrusion
and pelletizing of waste films, results in a colour change.
3.2. Stress and strain at rupture
Stress at rupture (MPa) was studied for the materials reported
(Fig. 2). For the LLDPE films, an increasing trend was seen with
V/W (100/0)
exposure duration followed by a sharp decline in stress. This was
V/W (75/25)
expected and reported previously for virgin polymers [18,21,22],
V/W (50/50) and is typically related to the cross-linking of LLDPE in the initial
stages of weathering, as well as the molecular weight reduction
V/W (25/75)
leading to the loss of mechanical integrity, which was observed
V/W (10/90) after about 70 h of weathering. The 75/25 (wt.%/wt.%) blend
300 350 400
with no weathering. A severe decline was observed by comparison
for the virgin LLDPE samples (<30%), especially after 200 h of
exposure. The cross-linking phenomenon was clearly taking effect
on the LLDPE at this stage, which can be observed from the slight
drop in the modulus and recovery in stress at rupture (Figs. 1e2).
Generally, the increase in waste content in the blend results in a
stress at rupture reduction (Fig. 2). However, the 90/10 (wt.%/wt.%)
blend showed a higher performance compared to other blends. This
indicates that adhesion and binding problems are least exhibited in
a blend with one dominant material in its formulation, which in
this case will be the LLDPE from both the virgin resin and the PSW
used. Several authors have shown strain and elongation at rupture
to be a very useful measurement of polymer degradation
[7,9,23,24]. It was noted that the values of strain at rupture for
LLDPE dropped to 25% of the initial value, with a continuous drop
until reaching values near zero (Fig. 3). A similar trend was
observed for the other tested materials. This behaviour can be
related to chain scission in semi-crystalline polymers which leads
to a decrease in the molecular weight of the material and, conse-
quently, a loss in strain and elongation at rupture with weathering
[7,24,25,26]. Strain at rupture followed a decreasing trend propor-
tional to waste material content as seen in Fig. 3.
3.3. Force at rupture
Force at rupture was monitored for the studied materials and
reported in Fig. 4. A decrease in measured force was observed with
increasing waste content. The force at rupture indicates the integ-
rity of the polymer along with other mechanical properties. Virgin
LLDPE showed comparable results to 75/25 (wt.%/wt.%) samples
with no exposure. Similar observation was noted for the 50/50 and
25
V/W (100/0)
V/W (75/25)
20
V/W (50/50)
V/W (25/75)
Stress at rupture (MPa)
15
V/W (10/90)
10
5
0
0 50 100 150 200 250 300 350 400
Exposure Duration (Hours)
Fig. 2. Stress at rupture (MPa) as a function of accelerated weathering duration
(hours).
 S.M. Al-Salem et al. / Polymer Testing 46 (2015) 116e121 119

1600
V/W (100/0) V/W (75/25) V/W (50/50) V/W (25/75) V/W (10/90)
50
1400
45
1200

40
1000
Strain at rupture (%)

35
800

Haze (%)
600 30

400 25

200 20

0
15
0 50 100 150 200 250 300 350 400
0 50 100 150 200 250 300 350 400
Exposure Duration (Hours) Exposure Duration (Hours)

Fig. 3. Strain at rupture (%) as a function of accelerated weathering duration (hours). Fig. 5. Haze (%) measured as a function of exposure time (hours).

92.0
10/90 (wt.%/wt.%) blends, with the 25/75 (wt.%/wt.%) showing the V/W (100/0) V/W (75/25) V/W (50/50) V/W (25/75) V/W (10/90)
lowest measured force at the breaking point (Fig. 4). The domi- 91.8
nance of a material, whether the virgin LLDPE or the waste, gives 91.6
compatibility to the results. This indicates that developing a
91.4
product from these blends utilizing mechanical recycling is mate-
rial sensitive and could be altered according to the intended 91.2
Transmission (%)

application. It can be seen from the trend of the 10/90 (wt.%/wt.%)

91.0
blend that it is superior to the 25/75 (wt.%/wt.%) films. This shows
that the force required for material rupture is dependent on one 90.8

type of resin used, in this case the virgin or the waste which was 90.6
pelletized and treated as a standalone material in the blending and
90.4
compounding process. The presence of stabilisers and other addi-
tives originating from the waste material used could be the reason 90.2

behind the requirement of a high force to rupture the samples, 90.0

incrementally increasing with the content of waste material. This 0 50 100 150 200 250 300 350 400

was also observed by comparing the results of this study to pre- Exposure Duration (Hours)
vious work [12,18] with a similar duration of threshold limit in
Fig. 6. Transmission (%) measured as a function of exposure time (hours).
accelerated weathering.

3.4. Haze and transmission

blends, the haze increasing with exposure to weathering, showing
an increase of about 10% by the end of the weathering time (Fig. 5).
Haze and transmission are the two key optical properties typi-
The loss of amorphous regions with degradation causes the loss of
cally measured in polymer films [27]. Haze of polymer films can be
clarity and an increase in haze. The compatibility of the samples
caused due to surface irregularities due to the effects of degradation
with blending is a major factor in polymer haze measurements. A
[28]. Virgin LLDPE proved to become more hazy than the other
notable reduction in the measured haze (%) when altering the
waste content was observed. The inclusion of different types of
polymers in the blends tested stabilises the haze measured, and the
30 V/W (100/0) effect of weathering was not observed to be of significance (Fig. 5).
This could be attributed to binding issues at the extrusion stage
V/W (75/25)
with no addition of chemicals or additives. However, measured
25
V/W (50/50) light transmission (%) showed a gradual decrease with exposure
V/W (25/75) time (Fig. 6). Comparatively, the 10/90 (wt.%/wt.%) formulation was
20 clearly showing the least transmission among the tested materials.
Force at rupture (N)

V/W (10/90)
This indicates a lack of compatibility in the blend's polymer matrix
15

Table 1
10
Control samples (no exposure) colour parameters.

Materials (wt.%/wt.%) L*s a*s b*s

5
0 50 100 150 200 250 300 350 400 LLDPE/Waste (100/0) 29.0 0.4 3.5
LLDPE/Waste (75/25) 25.2 0.4 4.8
LLDPE/Waste (50/50) 23.0 0.6 5.9
Exposure Duration (Hours)
LLDPE/Waste (25/75) 20.1 0.5 5.6
LLDPE/Waste (90/10) 18.0 0.4 5.5
Fig. 4. Force at rupture (N) as a function of accelerated weathering duration (hours).
120 S.M. Al-Salem et al. / Polymer Testing 46 (2015) 116e121

Table 2
Colour parameters and total change in colour (DE) for studied formulations at different accelerated weathering exposure (hours).

Materials (wt.%/wt.%) Exposure duration (hours) L*s a*s b*s DE Materials (wt.%/wt.%) Exposure duration (hours) L*s a*s b*s DE
LLDPE/Waste (100/0) 48 27.0 0.7 4.5 2.2 ± 0.1 LLDPE/Waste (75/25) 48 26.4 0.7 3.8 1.4 ± 0.5
72 26.6 0.2 4.3 2.5 ± 0.2 72 24.4 0.1 6.4 1.8 ± 0.2
120 26.0 0.3 4.5 3.3 ± 0.1 120 26.4 0.1 5.6 1.8 ± 0.1
168 28.6 0.3 3.9 0.6 ± 0.4 168 26.1 0.3 5.6 1.2 ± 0.3
216 26.1 0.1 4.2 3.0 ± 0.3 216 26.5 0.4 5.2 1.2 ± 0.2
264 29.1 0.04 4.0 0.6 ± 0.4 264 28.2 0.1 5.0 3.0 ± 0.1
360 28.5 0.07 3.9 0.8 ± 0.1 360 26.8 0.05 5.0 1.7 ± 0.1
LLDPE/Waste (50/50) 48 28.6 0.7 7.0 5.7 ± 0.8 LLDPE/Waste (25/75) 48 22.4 0.5 5.4 2.3 ± 0.3
72 26.6 0.3 6.6 3.7 ± 0.1 72 22.2 0.1 6.2 2.2 ± 0.1
120 24.5 0.1 6.5 1.7 ± 0.3 120 21.3 0.1 6.0 1.3 ± 0.4
168 22.2 0.2 6.0 2.1 ± 0.1 168 21.8 0.2 6.2 1.8 ± 0.1
216 24.4 0.2 6.0 1.5 ± 0.1 216 22.2 0.2 6.0 2.1 ± 0.1
264 28.2 0 6.2 5.3 ± 0.1 264 24.2 0.05 6.3 4.1 ± 0.2
LLDPE/Waste (10/90) 48 19.0 0.5 6.2 1.1 ± 0.3
72 19.0 0.5 6.2 1.1 ± 0.2
120 20.2 0.1 5.9 2.2 ± 0.2
168 19.8 0.2 5.7 1.7 ± 0.2
216 19.3 0.1 5.7 1.2 ± 0.2
264 19.0 0.1 5.7 1.1 ± 0.2

which is attributed to the chemical immiscibility of the constituting
materials. Hence, films of this formulation present a superior ma-
terial for cover applications, especially in sunny climates.
3.5. Total change in colour (DE)
this research project (PC017C). Mr. M. Al-Mujaibel and A. Al-
Marshad are graciously acknowledged for their support of this
work. Dr. A.Tuhl's (NWM Co. Kuwait) contribution is appreciated at
the start of this work. Comments from Dr. F. Rasoul and Dr. A. Yussuf
(PRC-KISR) are appreciated.

Control specimen measurements are shown in Table 1, and the References

total change in colour (DE) was estimated with respect to different
weathering durations and presented in Table 2. Gloss and colour
loss are affected by UV exposure. The estimated total change in
colour (DE) for the materials studied did not show a clear trend
with respect to weathering time (Table 2). Dehbi et al. [29] indi-
cated that the change in colour was related to washing due to water
spray and rain in weathering, making colour change a continuous
process during the weathering exposure time. In this work, there
was no trend that could be observed in estimated DE. However, a
continuous change in the colour parameters was seen. This could
be related to loss of dye from waste material or a UV chamber water
wash mechanism, which could affect the colour measurements.
4. Conclusions
Various formulations of virgin LLDPE blends with plastic waste
films were studied in this work and the effect of accelerated
weathering on the mechanical and physical properties measured
after different durations of accelerated weathering exposure. The
Young's modulus was observed to increase with weathering dura-
tion, which is possibly related to alterations in the samples' crys-
tallinity. It was seen that a cross-linking effect was involved during
stress at rupture measurements due to polymer degradation, with a
disproportional effect on the increase in waste content in the tested
blend samples. The physical properties studied (i.e. haze and light
transmission (%)) were sensitive to weathering. The loss of amor-
phous regions was suspected to cause the decrease in transparency
and increase in the haze of samples. The total change in colour
estimated for the tested polymer blends did not show a clear trend.
This could be the result of the continuous degradation mechanisms
and weathering test conditions.
Acknowledgments
The Kuwait Institute for Scientific Research (KISR) and EQUATE
Petrochemical Company are gratefully acknowledged for funding
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