Research Article

Nanomaterials and Nanotechnology

Volume 7: 1–11
ª The Author(s) 2017
Influence of mechanical properties of DOI: 10.1177/1847980417715929
journals.sagepub.com/home/nax
polypropylene/low-density polyethylene
nanocomposites: Compatibility
and crystallization

Bei Su1, Ying-Guo Zhou1, and Hai-Hong Wu2

Abstract
The mechanical blending of polypropylene and low-density polyethylene is an economical and simple method for pro-
ducing new polymeric materials for specific applications. However, the reduction in mechanical properties of the blend is
one of its main shortcomings. In this study, a filler masterbatch including nano-silicon dioxide, compatibilizer, lubricant
agent, and antioxidant agent was prepared, and polypropylene–low-density polyethylene composite parts with different
content of filler masterbatch were fabricated and tested for mechanical properties at two tensile test speeds. Also, to
investigate the underlying mechanism of the mechanical properties improvement, the tested samples were carefully
analyzed and compared and further characterized by scanning electron microscopy and differential scanning calorimetry.
The results indicate that the mechanical properties, including tensile strength, moduli, and elongation, can be all drastically
improved simultaneously with the addition of the filler masterbatch. The results also suggest that the compatibility of the
two phases increases with the increase in the filler masterbatch, and the crystal size decreases and distribution uniforms
owing to the addition of the filler masterbatch. Furthermore, it was also found that there is a close relationship between
the mechanical properties and morphological structures, which are improved by the existence of the filler masterbatch.

Keywords
PP/LDPE, nanoparticles, compatibilizer, mechanical properties

Date received: 14 February 2017; accepted: 8 May 2017

Topic: Nanocomposites, Nanophase Materials and Nanoscale Characterizations

Topic Editor: Leander Tapfer
Associate Editor: Halima Alem-Marchand

Introduction components.4–8 Furthermore, with their more similar chem-

Polypropylene (PP) and low-density polyethylene (LDPE)
are both widely used polyolefin polymers owing to their
advantages such as low density, high stiffness, high soften-
ing temperature, and good chemical inertness. More impor-
tant, in addition, is the cheapness and ease with which they
can be processed. The mechanical blending of PP and LDPE,
if they result in a combination of the mechanical perfor-
mance of both components, may prove to be a more eco-
nomical and easier method for producing new polymeric
materials for specific applications.1–3 In the past decade,
high volume commodity PP and LDPE have been blended
in hopes of combining the mechanical performance of both
ical structures, the possibility of recycling plastic waste—
mainly constituted by polyolefins9,10—and avoiding the
1
School of Material Science and Engineering, Jiangsu University of Science
and Technology, Zhenjiang, Jiangsu, People’s Republic of China
2
School of Materials Science and Engineering, Henan University of
Technology, Zhengzhou, Henan, People’s Republic of China
Corresponding author:
Ying-Guo Zhou, School of Material Science and Engineering, Jiangsu
University of Science and Technology, Zhenjiang, Jiangsu 212003,
People’s Republic of China.
Email: zhouyingguo@gmail.com

Creative Commons CC BY: This article is distributed under the terms of the Creative Commons Attribution 4.0 License
(http://www.creativecommons.org/licenses/by/4.0/) which permits any use, reproduction and distribution of the work without
further permission provided the original work is attributed as specified on the SAGE and Open Access pages (https://us.sagepub.com/en-us/nam/
open-access-at-sage).
2 Nanomaterials and Nanotechnology
complex and expensive processes of separation of the dif-
ferent components have been investigated. Generally, blend-
ing PP and PE yields properties in between those of the
original homopolymers. However, the main shortcoming
of the blends is the drastic reduction in toughness and elon-
gation at break.4,5 Hence, for the successful application of
PP–LDPE blends, improvement in toughness and elongation
at break is important.
It is generally believed that the compatibility is an
important influencing factor on the mechanical properties
of polymer blends. For PP and LDPE, it has also been
proven that they are incompatible in the melt, and the blend
exists as a two-phase mixture.11 Therefore, adding compa-
tibilizers is often viewed as a conventional method to
improve the poor interfacial bond strength between both
phases of polymer blends.12 There have been many elasto-
mers proven to be effective for PP–LDPE blends, for exam-
ple, styrene-butadiene-styrene,13 ethylene-propylene-diene
rubber,14 ethylene-propylene-ethylidene norborene copoly-
mer (EPCAR-847),15 PE-g-poly(2-methyl-1,3-butadiene),9
and so on. In addition, one can introduce micro or nano-
particles—such as talc,16 carbon nanotube,17 nanoclay,18
nano-silicon dioxide (nanoSiO 2),19 nanoTiO 2,20 SiO2/
TiO2,21 and cellulose nanofibers22—into the blended mate-
rial to enhance the mechanical properties of a component
fabricated by polymer or polymer blends. However, it was
often reported that tensile strength, elastic modulus, and
stress at break of the blends with a compatibilizer or nano-
filler decreased while impact strength and elongation
increased and vice versa. This motivated us to explore other
methods of improving the mechanical performances
including the strength and elongation simultaneously of
PP–LDPE blends.
Considering the role of nanofillers and compatibilizers
in the enhancement of mechanical performances of poly-
mers, it is expected that the appropriate addition of nano-
fillers and compatibilizers into a PP–LDPE blend system
may have a synergistic effect and further improve its
strength and elongation. In this study, a method of introdu-
cing both nanoparticles and compatibilizers into PP–LDPE
blends, which could produce counterparts with improved
strength and elongation simultaneously, was introduced,
and the influences of compatibilizer and filler content on
the structure–property relationship were carefully com-
pared. A better understanding of the properties-enhancing
mechanism was gained from the results and from compar-
isons with common blended parts.
Experimental work
Materials
The PP (Huajin T30 S) and LDPE (Maoming 951-000)
used in this study were commercial products made in
China. Their melt flow indexes were about 3.2 g/10 min
(190 C, 21.6 N) and 2.17 g/10 min (230  C, 21.6 N),
respectively. Ethylene-vinyl acetate copolymer (EVA) was
used for the carrier of the masterbatch. The content of vinyl
acetate was about 28.0 wt%. PP-graft-maleicanhydride
(PP-g-MA) with a graft ratio of 8.0 wt% was used for the
compatibilizer. It was supplied by Sigma-Aldrich Co., Ltd,
St. Louis, USA, and its melt flow index was about 5 g/10
min (190 C, 21.6 N). Polyethylene wax (H1001) and hin-
dered phenolic (B225/1010) were used as a lubricant and
antioxidant agent, respectively. The nanoSiO2 with average
radius of 5 nm was used for a nucleating agent. All the
materials were strictly selected after a series of experiment
and comparison, and the screening procedure was omitted.
Sample preparation
Sample preparation could be mainly classified into two
stages, filler masterbatch (FM) preparing and sample pro-
cessing. The FM preparing stage was realized in three
steps. First, all the materials were dried and weighted. Sec-
ond, the components of the FM, including EVA, PP-g-MA,
nanoSiO2, H1001, and B225/1010, were blended using a
high-speed mixer, and the weight ratio of EVA, PP-g-MA,
nanoSiO2, H1001, and B225/1010 was kept as 60:18:20:1:1
for brevity. Finally, the mixed materials were melted and
extruded through a F3-mm filament die by a two-screw
extruder (SHJ-30, Nanjing Keya Machinery Co., Ltd,
China). The extruded material was cooled down once
exited from the die and then pelletized using a QLJ-300
pelletizer. Some key processing parameters of the FM
fabrication are listed in Table 1.
Once the FM was prepared, PP, LDPE, and the pelle-
tized FM can be mixed for the next sample fabrication. For
brevity, the weight ratio of PP–LDPE was fixed on 3:1. As
to the FM, its content varied across a range of 5–15 wt%,
depending on the process used. As a result, the nanoSiO2
content in the PP–LDPE–FM composite was 1.0–3.0 wt%.
Using the conventional sample without the FM for compar-
ison, there were four FM sample formulations by weight:
0%, 5.0%, 10.0%, and 15.0%, and the nanoSiO2 contents
were 0%, 1.0%, 2.0%, and 3.0%, respectively. The four
kinds of sample were named as PLN0, PLN1, PLN2, and
PLN3, respectively. The detailed content of the four sam-
ples are listed in Table 2. The sample was then fabricated
using the different PP–LDPE–FM composites in a conven-
tional injection molding (CIM) machine (HTF-80, Ningbo
Haitai Co., Ltd, China). For comparison, PP–LPDE–EVA,
PP–LDPE–PP-g-MA, and PP–LDPE–nanoSiO2 samples
were also prepared by a direct procedure of mixing. For
being close to PLN3, the ratios of their composition
were fixed as 67.82:22.61:9.57, 72.69:24.23:3.08, and
72.44:24.15:3.41, respectively.
It should be noted that the dispersity of the nanoSiO2 in
the stage of FM preparation is a very important influence
factor to determine mechanical properties of the compo-
sites. The distribution of nanoSiO2 in PLN3 and PP–
LDPE–nanoSiO2 samples were first investigated by the
Su et al. 3

Table 1. Processing parameters of the FM fabrication.

Processing condition Speed of screw rotation Temperature of hopper Temperature of die Speed of take-up rolls
 
Value 60 rpm 110–130 C 125 C 1.2 m/s
FM: filler masterbatch.

Table 2. Materials used for processing samples of PP–LDPE composites.

Weight ratio Weight ratio Weight ratio Weight ratio

Function Material Designation (%) in PLN0 (%) in PLN1 (%) in PLN2 (%) in PLN3
Polymer matrix PP T30S 75 71.25 67.5 63.75
Polymer matrix LDPE 950-001 25 23.75 22.5 21.25
Carrier EVA 0 3 6 9
Compatibilizer PP-g-MA 0 0.9 1.8 2.7
Nucleation agent nanoSiO2 Radius of 5 nm 0 1 2 3
Lubricant agent Polyethylene wax H1001 0 0.05 0.1 0.15
Antioxidant agent Hindered phenolic B225/1010 0 0.05 0.1 0.15

PP: polypropylene; LDPE: low-density polyethylene; EVA: ethylene-vinyl acetate copolymer; PP-g-MA: PP-graft-maleicanhydride.

Figure 1. Comparison of the distribution of the nanoSiO2 in PLN3 (a) and PP/LDPE/nanoSiO2 (b) using SEM observation. nanoSiO2:
nano-silicon dioxide; PP: polypropylene; LDPE: low-density polyethylene; SEM: scanning electron microscope.

following scanning electron microscope (SEM) observa-
tion, and the results are shown in Figure 1(a) and (b),
respectively. It is easily found that the nanoSiO2 can be
distributed in the PP–LPDE matrix more uniformly in the
PLN3 sample compared to the PP–LDPE–nanoSiO 2
sample. Therefore, the EVA used in this study not only
helps to increase the compatibility of PP and LDPE owing
to its structure but also is a good carrier. It also actually
functions as a dispersion agent.
The conventional procedure of injection molding is well
known. First, the raw material is heated to its melting tem-
perature. By high pressure, the melted polymer is injected
into the cavity via a delivery system and a gate. When
filling is nearly completed, the cavity is maintained at a
constant pressure for the packing stage. Packing pressure is
used to fill the remaining volume of the cavity and to com-
pensate for shrinkage in the cooling stage, the shrinkage
results in the decrease of the dimensions as the cavity cools
down. After the interior of cavity has become stable, the
product is ejected from the mold. It is also well known that
defects of the products, such as warpage, shrinkage, sink
marks, and so on, are caused by many factors during the
production process. These defects influence the quality and
accuracy of the products. Therefore, it is of critical impor-
tance to effectively control the factors of influence during
the molding procedure. The processing parameters during
the injection molding mainly include melt temperature,
mold temperature, injection pressure, injection time (rate),
packing pressure, packing time, and cooling time. After
many tests, the optimal processing parameters were
obtained as follows: injection machine melt temperature
of 200 C, mold temperature of 50 C, injection pressure
of 60 MPa, injection time of 1 s, packing pressure of 70
MPa, packing time of 5 s, and cooling time of 20 s. As such,
it was still difficult to avoid the shrinkage of the molded
samples owing to the high crystallinity of the raw materials
4 Nanomaterials and Nanotechnology
Figure 2. A detailed description of the preparation of the molded sample.
(PP and LDPE). A standard tensile test bar mold was used
to mold the parts, and its temperature was controlled by
circulating oil from a thermal controller. The volume of the
cavity was about 9.582  103 mm3, and a detailed descrip-
tion of the molded sample is shown in Figure 2. According
to the volume of the cavity, a shrinkage rate of volume
could be calculated for all the molded samples. It was
found that the shrinkage rate of volume has a slight increase
with the increases in the FM. The shrinkage rate of volume
for PLN0 sample is about 3.78% and that of PLN3 is about
4.02%. It was possibly owing to the variation in the crystal-
lization with the addition of the FM.
Sample test
The molded tensile bars were tested on a screw-driven universal
testing instrument (MTS, Sintech 10/GL, MTS Systems Corpo-
ration, Eden Prairie, USA) per ASTM D638-03 at a room tem-
perature of 25 C. Two crosshead speeds, 10 and 500 mm/min,
were used to study the stress and strain behavior. At each test
speed, seven tensile bars were tested for each material, and five
values were selected and analyzed excluding the biggest and the
smallest values. The mean and range of the modulus of elasticity
(Young’s modulus), ultimate tensile strength, and strain at break
for each group sample were calculated. In this study, the tensile
strength was nominal, and it was obtained by dividing the load
by the original cross-sectional area.
The morphologies of the selected molded specimens were
first examined using an SEM (JEOL JSM-6480) with an
accelerating voltage of 20 kV. The SEM specimens were
taken from the cross-section at the middle of the molded
tensile bar (shown in Figure 2) which was fractured in liquid
nitrogen. The surfaces of the fractured specimens were sputter
coated with gold prior for a period of 50 s to observation using
a Cressington 108Auto sputter coater (Cressington Scientific
Instruments Ltd, UK). To better characterize the morpholo-
gical distribution in the molded samples, the fractured sur-
faces were chemically etched and then also observed using a
field emission SEM (JEOL JSM-7100F) with an accelerating
voltage of 10 kV. Etching was used to remove the noncrystals
material and get to know the distribution of crystals. The
etchant used was a solution of potassium permanganate in a
mixture of 10:4:1 by volume of concentrated sulfuric acid,
phosphoric acid, and distilled water (1 g of potassium per-
manganate in 100 ml of mixture). The etching lasted for 6 h at
a temperature of 60 C, and it partially revealed the surface
topography. After that, the etched surfaces were washed,
dried, and covered with a thin layer of gold.
A Perkin–Elmer DSC-8000 (Waltham, USA) apparatus
was used to analyze the thermal properties of the selected
samples with a series of procedures. The temperature was
calibrated with indium. All differential scanning calorime-
try (DSC) sample weights were strictly limited in the range
of 4.9–5.1 mg in order to avoid the possible influence of the
sample size. Samples were loaded to the DSC at 25 C, and
liquid nitrogen was used as the cooling fluid. The samples
were heated to 240 C and kept at this temperature for 3 min
to eliminate any residual crystals and prior thermomecha-
nical history. Then, they were cooled to 60 C and kept for 3
min. Finally, the samples were reheated to 240 C. For
brevity, all of the heating/cooling rates were fixed at
10 C/min.
Results and discussion
Mechanical properties
Tensile tests were performed on the injection molded speci-
mens of PP–LDPE nanocomposites. Properties such as the
Su et al.
Figure 3. A comparison of tensile strength and strain-at-break of
the molded PP/LDPE sample with different composition (tensile
rate of 10 mm/min). PP: polypropylene; LDPE: low-density
polyethylene.
strength, modulus, and strain at break were measured. PP–
LPDE–EVA, PP–LDPE–PP-g-MA, PP–LDPE–nanoSiO2,
and PLN0 samples mentioned before were first investi-
gated by the tensile test. The results of the tensile strength
and the strain at break at the tensile speed of 10 mm/min
were shown in Figure 3. It can be seen from Figure 3 that
the tensile strength and the strain at break are almost equiv-
alent to the PP–LDPE–PP-g-MA, PP–LDPE–nanoSiO2,
and PLN0 samples, which suggests that the effect of the
separate PP-g-MA and nanoSiO2 on the mechanical prop-
erties of PP–LDPE blends is less significant. As to the PP–
LDPE–EVA sample, which has a relatively low tensile
strength and high strain-at-break compared to that of the
PLN0 sample, it indicates that the elongation increases
and the strength decreased with the addition of EVA. It
is possibly attribute to the low strength of EVA and the
enhancing compatibility of PP and LDPE owing to the
existence of EVA. It can be concluded from these results
that one single composition of EVA, PP-g-MA, and nano-
SiO2 has less influence on the mechanical properties of
PP–LDPE blends.
However, the EVA, PP-g-MA, and nanoSiO2 have a
synergistic effect on the improvement in the mechanical
properties of PP–LDPE blends. Figure 4 shows an illustra-
tive comparison of the tested samples at the tensile speed of
10 mm/min. For the neat PP–LDPE blended parts—those
with an FM content of 0 wt%—yielding and then necking
were observed to occur. However, the necking only lasted a
short distance and then the part ruptured (Figure 4(b)). For
the filled parts, the necking spread and measured several
hundred percent strain. As the FM content increases, the
necking can spread more smoothly. When the FM content
was 15.0 wt% (PLN3, Figure 4(e)), the necking can spread
throughout all the gauge length. As a result, a 650% elon-
gation can be found and the sample is not actually ruptured
(exceeds the limits of the experimental apparatus). This
deformation behavior is similar to typical semicrystalline
5
polymers capable of undergoing chain orientation. An
interesting phenomenon can also be observed from Figure
4 in that a lot of threadlets (small thread- or hair-like pro-
trusions) formed on the surface of the samples with 15.0-
wt% FM content. The more ductility the sample had, the
rougher the surface was, and the more threadlets were
found. It is possibly attribute to a small portion of surface
material separate from the kernel and break in advance
owing to the heat release in the last stage of the tensile test.
Figure 5 shows the representative engineering stress–
strain curve of the four samples at a test speed of 10 mm/
min. From Figure 5, one can clearly see that the PLN3
sample exhibits the more ductile fracture characteristics
than the PLN2, PLN1, and PLN0. Especially, apart from
regions including the elastic region, yield point, stress drop
region, cold drawing, and fracture point can be observed in
all these curves, the strain hardening region is easily found
after 450% strain of the PLN3 sample. Furthermore, the
tensile strengths and moduli are also found to be increased
with increasing the FM content. The results are in agree-
ment with the results shown in Figure 4, and it can be
attributed to the presence of the FM.
For further comparison, the results of tensile strength,
strain at break, and moduli of the samples with different
amounts of FM are shown in Figure 6. The properties
reported here are the actual readings measured for the spe-
cimens without taking into account the variation in the
sectional dimension and slight elongation after rupture. It
can be seen from the figure that the tensile strengths, strain
at break, and Young’s moduli of the samples with filled FM
are all higher than the unfilled ones. Therefore, it can be
concluded that the filled samples had better mechanical
properties than the unfilled ones. Furthermore, with an
increase in FM content, the tensile strengths, strain at
break, and Young’s moduli of the filled samples all obvi-
ously increased. The best result of the mechanical proper-
ties occurred when the FM content was 15.0 wt% and
showed approximately 25.2-MPa tensile strength, 650%
strain-at-break, and 1270-MPa Young’s modulus.
It must be noted that the tensile test could not stop
immediately when the samples were partially fractured
owing to a small portion of material still keeping unbroken
at the low-speed tensile test (10 mm/min). As a result, the
tested value of the strain-at-break may be influenced by the
delay. Hence, in order to examine the energy required to
perform tensile testing until rupture more exactly, a tensile
speed as high as 500 mm/min, which is the upper limit of
the testing equipment, was also used to determine the
stress–strain behavior of the different molded samples.
As can be seen from Figure 7, four representative stress–
strain plots were selected for comparison among samples
with different amounts of FM. For the filled and unfilled
parts, no matter what the FM content was, yielding was first
observed at approximately 10% strain. Necking took place
next. It should be noted that high-speed tensile tests have a
different effect on samples when compared to low-speed
6 Nanomaterials and Nanotechnology
Figure 4. Pictures of the molded sample with different amounts of FM before and after the tensile test. (a) Untested sample. (b) to (e)
Tested samples. The scale bar is 100 mm. (f) and (g) The magnification of the picture (b) and (d). FM: filler masterbatch.
Figure 5. Representative tensile stress versus strain of the
molded sample with different amounts of FM (tensile rate of 10
mm/min). FM: filler masterbatch.
tests. In a high-speed test, the necking doesn’t have enough
time to spread and cold drawing is difficult, so cracks pro-
pagate rapidly. Hence, the high-speed tensile test is a good
way to measure the energy required to perform tensile test-
ing until rupture of a part. As a result, it can be concluded
that the longer the necking lasts, the better the ductility is.
Thus, from Figure 7, it can be seen that the filled parts had
better ductility than the unfilled ones and that the parts with
15.0-wt% FM performed the best.
For convenient comparison, the following integral
expression of the stress–strain curve was used to describe
the energy required to perform tensile testing until rupture
quantitatively
εðb
E ¼ τdε (1)
0 more completely.
where τ is the apparent tensile stress, ε is the corresponding
tensile strain, and εb is the strain at break. As a result, the
integral value is symbolized as E, and the units are kilo-
joule/cubic meter. This result is similar to the tensile impact
strength except that the speed of the tensile test used in this
study was still lower than that of the standard tensile impact
test as specified in the ASTM-D1822. Hence, the data were
simply used here as a direct comparison among all foamed
samples. In general, the higher the integral result is, the
more ductile the tested sample is. According to equation
(1), the result of the four stress–strain curves is listed in
Table 3. As shown in Table 3, the highest value calculated
was 1182.71 KJ/m3, corresponding to the most ductile sam-
ple with a filler content of 15.0 wt%.
A conclusion can be drawn from the above experimental
results and discussion. For the PP–LDPE 3:1 composites,
the presence of the FM presented in this study can help to
drastically improve the mechanical properties, which
include strengths, strain at break, and moduli, simultane-
ously. Furthermore, the mechanical properties increase
with increasing the FM content within limits. This demon-
strates the reinforcement effect of the filler on the PP–
LDPE composites.
However, it must be noted that the FM, which is mainly
comprised of EVA and PP-g-MA, has actually relatively
small tensile strength and modulus compared to the neat
PP–LDPE material. Hence, the dramatically increased
mechanical performance for the FM-filled samples remains
a mystery. For getting to be known it, the FM content was
further increased, and it was found that further increasing
the FM content could lead to the deterioration in tensile
performance. For example, when the FM content is 20
wt%, it was omitted for brevity, the tensile strength and
modulus of the sample will apparently show a low value
compared to that of the PLN2 sample, and almost the strain
at break of both is roughly the same. As a result, it is
necessary to clarify the mechanism of properties enhancing
Su et al.
Figure 6. The (a) tensile strength, (b) strain-at-break, and (c) Young’s modulus of the molded sample with different amounts of FM
(tensile rate of 10 mm/min). FM: filler masterbatch.
Figure 7. Representative tensile stress versus strain of the
molded sample with different amounts of FM (tensile rate of 500
mm/min). FM: filler masterbatch.
7
Relationship of morphology, structure, and
mechanical properties
The SEM is one of the most popular ways to identify
microstructural characteristics of the molded samples.
SEM images provide information on the microstructure,
including the phase morphology distribution and the frac-
ture characteristics of the specimens. Figure 8 shows rep-
resentative SEM images of the fractured surfaces of the
molded PP–LDPE composites with different amounts of
the FM. As can be seen in Figure 8, the increased misci-
bility of the PP and LDPE materials could be gradually
observed with an increase in the amount of the FM. In
Figure 8(a), the immiscibility can be clearly observable.
With an increase in the FM content, the phase dispersion
became gradually confused, as shown in Figure 8(b) and
(c). This suggests that the LDPE and PP were relatively
miscible with the addition of the FM. In Figure 8(d), the
FM content was 15.0 wt%, and the phase dispersion was
8 Nanomaterials and Nanotechnology

Table 3. Integral results of the stress–strain curves shown in Figure 6 and peak temperature values shown in Figures 9 and 10.

Integral value* PP crystallization peak LDPE crystallization peak PP melt peak  LDPE melt peak
Sample (KJ/m3) temperature** ( C) temperature** ( C) temperature*** ( C) temperature*** ( C)
PLN0 328.59 115.27 98.99 163.39 109.35
PLN1 514.15 116.22 98.04 162.79 109.95
PLN2 882.47 118.91 97.84 160.95 110.06
PLN3 1182.71 120.05 97.64 160.35 110.16
PP: polypropylene; LDPE: low-density polyethylene.
*
Integral results of the stress–strain curves shown in Figure 7.
**
Peak temperature values shown in Figure 10.
***
Peak temperature values shown in Figure 11.

Figure 8. SEM images of the molded sample. The FM content by weight was (a) 0%, (b) 5.0%, (c) 10.0%, and (d) 15.0%, respectively.
SEM: scanning electron microscope; FM: filler masterbatch.

difficult to determine. It can be concluded from the figure
that the presence of the FM has a great effect on the com-
patibility of the PP–LDPE composites, which greatly influ-
ences the micromorphological structure and mechanical
performance.
To better characterize the morphology structures of the
samples, the same slices analyzed by the previous SEM
were chemically etched according to the procedure
described in “Sample test” section and then also observed
using SEM. The resulting surface topography images are
shown in Figure 9.
The crystals dimension and distribution of the molded
samples with different FM content can be clearly observa-
ble from Figure 9. In Figure 9(a), for the neat PP–LDPE
binary blends, the crystals have an average radius of about
30 mm, and the distribution of crystals is not uniformed
relatively. With the addition of the FM, the crystals size
decreases obviously as shown in Figure 9(b) and (c). The
crystals shown in Figure 9(d) have an average radius of
about 20 mm, and further, almost all the crystals have the
same size, which suggests a uniformed distribution of
the crystals. This result was not unexpected and could be
Su et al. 9

Figure 9. SEM images of the etched sample. The FM content by weight was (a) 0%, (b) 5.0%, (c) 10.0%, and (d) 15.0%, respectively.
SEM: scanning electron microscope; FM: filler masterbatch.

attributed to the nucleating effect of the nanoSiO2. Up to

now, it is well known that nucleating agents of polymers
can fasten the crystallization and diminish the sizes of
crystals. Hence, the added nanoSiO2 could be concluded
to have contributed to improved crystallization behaviors
and mechanical properties of the PP–LDPE composites.
The different compatibilities and crystallization at dif-
ferent compositions of PP–LDPE composites can be further
characterized and verified by DSC testing, the results of
which are shown in Figures 10 and 11. As shown in Figures
10 and 11, although two distinct crystallization and melting
peaks can be seen in the curves of all of the composites—
thus indicating that the two phases of PP and LDPE are
strongly immiscible—the remelted peak (Figure 11) of PP
was shifted to the peaks of LDPE (Table 3) when the
amount of the FM was relatively high. According to Teh
et al.’s review,23 a simple and fast method to ascertain Figure 10. DSC curves of cooling after heating of the molded
compatibility is to run a DSC test on the blend to find out samples with different amounts of FM. DSC: differential scanning
whether there is any shift in melting points and/or change in calorimetry; FM: filler masterbatch.
enthalpy of fusion. Therefore, a conclusion can be con-
cluded that the LDPE and PP were relatively miscible with increases in the FM content. Furthermore, the crystallized
the presence of the FM. It is in agreement with the trend of peak (Figure 10) of PP was shifted to high temperature
the increased mechanical properties appeared with the with the addition of the FM, which indicated that the
10
Figure 11. DSC curves of second heating of the molded samples
with different amounts of FM. FM: filler masterbatch.
crystallization fastened owing to the nucleating effect of
the nanoSiO2. It can be concluded from the agreement
between the DSC and the SEM results that the mechan-
ical properties improvement can be attributed to the
improvement of the compatibilities and crystallization
of PP–LDPE composites, which is deeply influenced by
the presence of the FM.
Conclusions
In this study, the compatibility and crystallization, which
influenced by the compatibilizers and nanofiller, of PP–
LDPE composites parts molded by CIM were investigated.
It was found that the fabricated FM, which included nano-
SiO2, compatibilizer, lubricant agent, and antioxidant
agent, has the potential to improve the mechanical proper-
ties of PP–LDPE composites. In particular, tensile strength,
strain at break, and modulus can be enhanced simultane-
ously once the dosage of the FM is selected optimally. The
mechanism explaining the significant improvement in
mechanical properties of PP–LDPE composites parts by
CIM has been investigated, and it is proposed that the fun-
damental cause was the improvement in the compatibility
and the crystallization structures, which was determined by
the addition of the FM. Considering the advantages of the
FM method, such as easy storage and flexibly, it is believed
that the improvement in mechanical properties based on the
method suggested and proposed in this study—which only
depends on the dosage of the FM—is highly beneficial for
academic research and industrial application.
Declaration of conflicting interests
The author(s) declared no potential conflicts of interest
with respect to the research, authorship, and/or publication of
this article.
Nanomaterials and Nanotechnology
Funding
The author(s) disclosed receipt of the following financial support
for the research, authorship, and/or publication of this article: This
work was financially supported by the National Natural Science
Foundation of China (grant number 51373048), the Postgraduate
Research Innovation Program of Jiangsu University of Science
and Technology (grant number YCX16S-19), and the Postgradu-
ate Research and Practice Innovation Program of Jiangsu Prov-
ince (grant number KYCX17_1833).
References
1. Shanks RA, Li J, and Yu L. Miscibility and co-continuous
morphology of polypropylene- polyethylene blends. In: Pour-
deyhimi B (eds) Imaging and Image Analysis Applications for
Plastics: A volume in Plastics Design Library. Amsterdam,
Netherlands: Elsevier Publishing, 1999, pp.59–63. DOI: 10.
1016/B978-188420781-5.50009-7.
2. Paul DR and Newman S. Polymer blends. New York: Aca-
demic Press, 1978. ISBN: 978-1-884207-81-5.
3. Robeson LM. Applications of polymer blends: emphasis on
recent advances. Polym Eng Sci 1984; 24(8): 587–597.
4. Robertson RE and Paul DR. Stress–strain behavior of poly-
olefin blends. J Appl Polym Sci 1973; 17: 2579–2595.
5. Teh JW. Structure and properties of polyethylene-
polypropylene blend. J Appl Polym Sci 1983; 28: 605–618.
6. Liang JZ, Tang CY, and Man HC. Flow and mechanical
properties of polypropylene/low density polyethylene blends.
J Mater Proc Technol 1997; 66: 158–164.
7. Rizzo G and Spadaro G. Mechanical properties of low density
polyethylene-isotactic polypropylene blends: i. effect of mix-
ing time. Eur Polym J 1988; 24(4): 303–306.
8. Dong LS, Olley RH, and Bassett DC. On morphology and the
competition between crystallization and phase separation in
polypropylene–polyethylene blends. J Mater Sci 1998; 33:
4043–4048.
9. Mourad AHI. Thermo-mechanical characteristics of ther-
mally aged polyethylene- polypropylene blends. Mater Des
2010; 31: 918–929.
10. Bertin S and Robin JJ. Study and characterization of virgin and
recycled LDPE/PP blends. Eur Polym J 2002; 38: 2255–2264.
11. Malavasic T and Musil V. Thermal properties of binary poly-
olefin blends. Journal of Thermal Analysis, 1988; 34:
503–508.
12. Ha CS, Park HD, Kim Y, et al. Compatibilizer in polymer
blends for the recycling of plastics waste i: preliminary stud-
ies on 50/50 wt% virgin polyblends. Polym Adv Technol
1996; 7(5–6): 483–492.
13. Fortelný I, Kruliš Z, Michálková D, et al. Compatibilization
of polyethylene/poly(propylene)/polystyrene blends. Die
Angew Makromol Chem 1999; 270(1): 28–32.
14. Fortelný I, Kruliš Z, Michálková D, et al. Effect of EPDM
admixture and mixing conditions on the morphology and
mechanical properties of LDPE/PP blends. Die Angew
Makromol Chem 1996; 238: 97–104.
15. Barlow JW and Paul DR. Mechanical compatibilization of
immiscible blends. Polym Eng Sci 1984; 24(8): 525–534.
Su et al.
16. Fiorentino B, Fulchiron R, Duchet-Rumeau J, et al.
Controlled shear-induced molecular orientation and crystal-
lization in polypropylene-talc microcomposites – effects of
the talc nature. Polymer 2013; 54: 2764–2775.
17. Drdlova M, Frank M, Buchar J, et al. Effect of nanoparticle
modification on static and dynamic behaviour of foam based
blast energy absorbers. Cell Polym 2016; 35(3): 143–158.
18. Ibrahim MAH, Hassan A, Wahit MU, et al. Mechanical prop-
erties and morphology of polypropylene/poly(acrylonitrile-
butadiene-styrene) nanocomposites: effect of compatibilizer
and montmorillonite content. J Elastom Plast 2017; 49(3):
209–225. DOI: 10.1177/0095244316644859.
19. Qian J and Nie K. Non-isothermal crystallization of PP/Nano-
SiO2 composites. J Appl Polym Sci 2004; 91: 1013–1019.
11
20. Salehian H and Jenabali Jahromi SA. Effect of titanium diox-
ide nanoparticles on mechanical properties of vinyl ester-
based nanocomposites. J Compos Mater 2014; 49(19):
2365–2373.
21. Kang OL, Ahmad A, Hassan NH, et al. TiO2-SiO2-reinforced
methylated grafted natural rubber (MG49-TiO2-SiO2) poly-
mer nanocomposites: preparation, optimization and charac-
terization. Polym Polym Compos 2016; 24(9): 747–753.
22. Nakagaito AN, Kondo H, and Takagi H. Cellulose nanofiber
aerogel production and applications. J Reinf Plast Compos
2013; 32(20): 1547–1552.
23. Teh JW, Rudin A, and Keung JC. A review of polyethylene–
polypropylene blends and their compatibilization. Adv Polym
Technol 1994; 13(1): 1–23.