sustainability

Article
Extrusion Compounding Process for the Development
of Eco-Friendly SCG/PP Composite Pellets
Joo Seong Sohn , Youngjae Ryu , Chang-Seok Yun, Kun Zhu and Sung Woon Cha *
School of Mechanical Engineering, Yonsei University, 50, Yonsei-ro, Seodaemun-gu, Seoul 03722, Korea;
ssamjjang87@yonsei.ac.kr (J.S.S.); yjryu1027@yonsei.ac.kr (Y.R.); changseok2614@yonsei.ac.kr (C.-S.Y.);
hknuuz@yonsei.ac.kr (K.Z.)
* Correspondence: swcha@yonsei.ac.kr; Tel.: +82-2-2123-7224




Received: 15 February 2019; Accepted: 16 March 2019; Published: 21 March 2019


Abstract: As the consumption of coffee increases worldwide, the amount of spent coffee grounds
(SCG) is gradually increasing every year. Some of these grounds are recycled for composting, but most
are discarded, which causes widespread financial and social costs. We developed a bio-based plastic
pellet by blending polypropylene (PP) with waste biomass SCG to convert it into a sustainable,
recyclable eco-friendly material. It was confirmed that extrusion compounding for SCG/PP composite
pellets and injection molding with good formability are possible. To evaluate the formability of the
composite pellets, American Society for Testing and Materials (ASTM) test specimens were prepared
for evaluating mechanical properties by injection molding. As a result of the measurement of the
test samples, the mechanical properties of SCG/PP composite pellets were generally lowered as
the SCG content increased. However, the impact strength of SCG/PP composite based on the
HOMO-PP matrix improved as the SCG content increased. In addition, Young’s modulus of SCG/PP
increased as the SCG content increased. In the future, this study will be applied to manufacture of
products that requires non-toxic products, such as disposable products and food containers, realizing
commercialization of eco-friendly products and thereby replacing finite petroleum resources and
practicing resource circulation and environmental protection.

Keywords: spent coffee grounds; polypropylene; composites; extrusion compounding process;

injection molding process; mechanical properties

1. Introduction
Most common household items around us are made of plastic, which provides a lot of convenience
in our lives. However, since most conventional plastics are manufactured as disposable products, they
are not easily decomposed at the time of disposal, thereby causing environmental pollution and health
risk problems [1,2].
Since oil reserves in the earth are slowly depleting, it is necessary to reduce the use of petroleum
resources and develop alternative materials. In the long term, reducing the amount of plastics used
is an appropriate and practical method for reducing use of such resources. However, considering
the current industrial structures, such as production facilities, and demand in the market, it is almost
impossible to immediately stop using plastic materials. Therefore, we propose a realistic solution to
reduce the amount of plastic used, until the development of complete technology that does not use
plastic materials and the establishment of an improved industrial environment in the future.
In recent years, as the quality of life has improved and global environmental regulations have
emerged, there has been an increasing interest in environmentally friendly plastics to reduce emission
of carbon dioxide and to work toward carbon neutrality for green growth [3,4]. Many countries around

Sustainability 2019, 11, 1720; doi:10.3390/su11061720 www.mdpi.com/journal/sustainability

Sustainability 2019, 11, 1720 2 of 12

the world are actively pursuing research and technology development regarding environmentally
friendly bioplastics, and are preparing relevant laws and regulations.
Some of them are trying to increase the decomposition rate by reducing the amount of plastic and
by manufacturing bioplastics which are composite materials, including biomass from organic waste
resources [5,6]. As a concept of a quantitative biological resource, biomass is a renewable organic
resource. Examples of this include agricultural products such as sugar cane and starch, forest products
such as cellulose, microorganisms such as chlorella and spirulina, and whale oil. In other words,
all organisms are examples of biomass [7]. The total amount of biomass globally produced in one year
is similar to the total amount of petroleum produced, so it has the advantage of not being exhausted if
used appropriately [8,9]. A typical biomass material that has been in commercial use is wood. Many
studies have been carried out for manufacturing wood polymer composites by combining polymer
with wood [10–12]. In addition, studies on the addition of fly ash, which is generated in the process of
burning coal, to polymers have also been conducted [13–15].
From this viewpoint, we selected spent coffee grounds (SCG) as biomass and developed bio-based
plastic with an SCG content of more than 25% by an extrusion and injection molding process.
The manufacturing of SCG composites has been studied [16–19]. Chitra et al. analyzed the mechanical
properties of SCG/PP by incorporating 15% SCG into PP as a function of compatibilizer content by
extrusion and injection molding [16]. García-García et al. have found a difference in mechanical
properties of SCG/PP between the chemically pretreated SCG and the untreated SCG, when SCG
is added to PP at 20 wt % [17]. Essabir et al. identified the thermal, rheological, and mechanical
properties of SCG/PP composites as a function of SCG content (0~20 wt %) [19]. Although many
studies have been made on polymer composites with SCG, it has been difficult to satisfy the criteria for
being a bio-based plastic because its content is 20–25 wt % or less in extrusion and injection molding
process. Polymer composites, including biomass, can only be recognized as a bio-based plastic if the
biomass content exceeds 20–25 wt % (more than 20% in Europe, more than 25% in the United States,
Japan, and Korea) [20–22]. Our study is expected to provide a new recycling method for SCG.
As a foodstuff, coffee has a high weekly consumption rate per person. In addition, annual coffee
imports and coffee shops are on the increase, and the amount of SCG is also increasing. SCG is
classified as general waste and some is composted, but it is hardly utilized compared to the amount
of waste generated. This is because public awareness and interest in the recycling of SCG are not
high. Only around 0.2% of coffee beans are used to make coffee, and about 99.8% are discarded [23].
According to data from the International Coffee Organization, annual global coffee consumption has
grown to more than 100 million bags (1 bag = 60 kg) in recent years, and consumption is steadily
increasing as the coffee consumption population increases [24]. According to the report, by 2017,
Korea had become the seventh largest importer of coffee in the world. In Finland, the country with
the highest coffee consumption, people consume 12.5 kg of coffee per year on average. According to
the data from Statistics Korea (KOSTAT, Korea), as of 2014, around 270,000 tons of SCG were found
in sewage treatment plants [25]. SCG generates 50,490 tons of carbon dioxide per year and causes
environmental pollution. The cost of disposing of this waste is around $29 million, and the economic
loss, including labor costs, is around $680 million.
To solve the social disposal cost of SCG and to propose a new recycling plan, this study examined
the possibility of recycling SCG by developing eco-friendly bio-based high value-added plastic
composite pellets [26,27]. Bio-based plastics based on SCG can be recycled repeatedly after use,
and can be lightweight, save on manufacturing costs, and replace finite petroleum resources. Therefore,
resource circulation and environmental protection can be practiced.
Sustainability 2019, 11, 1720 3 of 12

2. Materials and Methods

2.1. Materials
HPP (HOMO-polypropylene, Lotte Chemical Corp., Grade No. J150, melting point—160 ◦ C,
density—0.9 g/cm3 , Seoul, Korea) and BPP (BLOCK-polypropylene, Lotte Chemical Corp., Grade
No. J350, melting point—160 ◦ C, density—0.9 g/cm3 , Seoul, Korea) were selected as the matrix of this
study and the SCG biomass was supplied from a coffee shop chain (Cafe Sharing, ANYONE F&C Co.,
Ltd., Seoul, Korea). The coffee beans were four varieties of Latin American beans, and the elapsed
time after roasting was within about two weeks (Table 1). The SCG were collected and dried at 90 ◦ C
for 12 h in a drier to remove moisture. Since SCG has a high water content after coffee extraction, mold
can grow if it is not dried properly. PP, a hydrophobic thermoplastic matrix, and SCG, a hydrophilic
natural material, were not compatible with each other. Therefore, compatibilizer was added to improve
the compatibility and interfacial adhesion between SCG and PP matrix. For compatibilizer, MAPP
(malleated polypropylene, Lotte Chemical Corp., Grade No. CM-1120W, Seoul, Korea) was added by
3 phr in the extrusion compounding process.

Table 1. The proportion of spent coffee grounds (SCG) collected in this study.

Coffee Bean Varieties Tarrazu Antigua Santos Medellin

Country of origin Costa Rica Guatemala Brazil Colombia
Mixing ratio (%) 20 30 20 30

2.2. Particle Size Classification Method of SCG

The SCG collected in this study are residual wastes remaining after coffee beans are pulverized
by a grinder (Super Jolly Electronic, MAZZER corp., Venezia, Italy). However, since the particle
size of the coffee bean was not easy to control given that the beans were ground in the coffee shop,
we attempted to single them out for uniform particle sizes. Uneven particle size adversely affects
the physical properties of the composite or final product, so the particle size must be checked and
should be uniformly controlled beforehand if necessary. Classification of the particle size was carried
out using a sieve test machine for 450 g of SCG, which shook the SCG for 300 s using a reciprocating
speed of 120 times per minute. The machine was made by our own laboratory, and the test sieve
(ChunggyeSieve Inc., Seoul, Korea) was purchased and fitted in the sieve test machine. The detailed
specification is shown in Figure 1 and Table 2. Sieves were arranged in a stack with the mesh number
in descending order from top to bottom. SCG clusters, which are clustered by residual moisture in
450 g of SCG, accounted for 4.4% (20 g) of the total amount. The particle size of 50 mesh was 36 g,
which accounted for 8% of the total, and the SCG corresponding to a particle size of 60 mesh was 4 g,
which was only 0.9% of the total. The average particle size of SCG was judged to be mainly in the
range of 30 to 40 mesh. SCG cluster, 50 and 60 mesh, which accounted for a relatively small proportion,
were excluded. Furthermore, the SCG cluster is likely to cause carbonization when it is discharged
from a nozzle during high-temperature, high-pressure extrusion and injection processes. Therefore,
the particle size of SCG selected in this study was in the range of 300–600 µm (Table 3 and Figure 2).

Table 2. Specification of sieve used in this study.

Vibratory Sieve Shaker

Number of mounted test sieves 7
Test sieve size (mm) 210(Φ) × 60(h)
Motor AC220 V, 60 Hz, 1/2HP
Operating method Shaking left and right
 Mesh number1 Cluster 30 40 50 60
Particle size (µm) Unknown 600 425 300 250
Amounts2 (g) 20 g 182 g (±21.0) 208 g (±16.0) 36 g (±5.2) 4 g (±3.2)
Ratio (%) 4.4 40.4 46.2 8.0 4
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1 Sieve 11, 1720
mesh chart for mesh number according to particle size based on ASTM E 11-70; 2 Sieve test for 4 of 12
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450 g of collected x FOR PEER REVIEW
SCG. 4 of 12

Table 3. Particle size distribution of collected SCG.

Classification of Particle Size for Collected SCG

Mesh number1 Cluster 30 40 50 60
Particle size (µm) Unknown 600 425 300 250
Amounts2 (g) 20 g 182 g (±21.0) 208 g (±16.0) 36 g (±5.2) 4 g (±3.2)
Ratio (%) 4.4 40.4 46.2 8.0 4
1 Sieve mesh chart for mesh number according to particle size based on ASTM E 11-70; 2 Sieve test for

450 g of collected SCG.

Figure1.1.Sieve
Figure Sieve test
test machine
machine designed
designedand
andused
usedininthis
thisstudy.
study.

Table 3. Particle size distribution of collected SCG.

Classification of Particle Size for Collected SCG

Mesh number 1 Cluster 30 40 50 60
Particle size (µm) Unknown 600 425 300 250
Amounts 2 (g) 20 g 182 g (±21.0) 208 g (±16.0) 36 g (±5.2) 4 g (±3.2)
Ratio (%) 4.4 40.4 46.2 8.0 4
1 Sieve mesh chart for mesh number according to particle size based on ASTM E 11-70; 2 Sieve test for 450 g of
collected SCG.
Figure 1. Sieve test machine designed and used in this study.

Figure 2. Results of classification experiments according to particle size of SCG collected by sieve
shaker.

2.3. Extrusion Compounding Process

Two types of matrix, HOMO-PP and BLOCK-PP, were used and compounding was performed
for SCG-PP composite material. PP and SCG were mixed in a weight ratio of 100/0, 90/10, 80/20, and
70/30 using an extruder (Yonsei University, Korea), and the mixture was poured into an extruder
hopper to form a composite material pellet (Figure 3). The screw was set at 120 rpm during the
extrusion compounding process. This is because, when compounding different kinds of materials, it
is desirable
Figure
Figure toResults
2. 2. have a of
Results high torque at experiments
of classification
classification a experiments
low speedaccording
foraccording
stabletodischarge,
to particle
particle but
size too
ofsize low
SCGof a discharge
SCG collected
collected speed
by sieve by
lowers
sieveproductivity.
shaker.
shaker. The heater temperature of the extruder was set at 200 °C. At lower temperatures,
feeding the material into the extruder barrel was difficult and the compounding did not work well.
2.3.Above
Extrusion
2.3. Extrusion
130 °C,Compounding
it was foundProcess
Compounding Process
that the temperature at which the discharge is performed while increasing
theTwo
molding
Twotypes temperature
types ofof
matrix, was
matrix,HOMO-PP smoothly
HOMO-PP andtransferred
and BLOCK-PP,
BLOCK-PP, at the
were
werereference
usedand
used temperature
and compounding
compounding of 200
was °Cperformed
was (Table 4).
performed
Temperatures
forfor
SCG-PP of
SCG-PPcomposite 200 °C
compositematerial.or higher
material. PP were
PP and
andSCG not considered
SCGwere
weremixed
mixed or
in inconfirmed
a weight
a weight through
ratio
ratio experiments.
of 100/0,
of 100/0, 90/10,90/10, As a
80/20, 80/20,
and
andbiomass,
70/30
70/30 usingSCG,
usingan anwhich
extruder is
extruder a natural
(Yonsei
(Yonsei material,
University,
University, can suffer
Korea),
Korea), andand from
thethe carbonization
mixture
mixture was was or
poured
poured clogging
into
into anan due to
extruder
extruder
caramelization
hopper
hopper to to formaofacomposite
form residual
compositesaccharides.
material The (Figure
material pellet
pellet compounding
(Figure Thedie
3). The waswas
screw
screw setset
was in aatcircle
setat 120rpm
120 shape
rpm withthe
during
during athe
extrusion
extrusion compoundingprocess.
compounding process. This
This is
isbecause,
because,when
whencompounding
compounding different kinds
different of materials,
kinds it
of materials,
it isisdesirable
desirable to have a high
high torque
torque at
ataalow
lowspeed
speedforforstable
stabledischarge,
discharge,butbuttoo low
too low a discharge
a dischargespeed
speed
lowers
lowers productivity.
productivity. Theheater
The heatertemperature
temperatureof of the
the extruder
extruder was
wasset
setatat200 ◦ C.
200°C. AtAt
lower temperatures,
lower temperatures,
feeding
feeding the
the materialinto
material intothe
theextruder
extruder barrel
barrel was
was difficult
difficultand
andthe
thecompounding
compounding did notnot
did work
workwell.
well.
Above 130
◦ °C, it was found that the temperature at which the discharge is performed
Above 130 C, it was found that the temperature at which the discharge is performed while increasing while increasing
thethe molding
molding temperaturewas
temperature wassmoothly
smoothly transferred
transferred atatthe
thereference
referencetemperature
temperature ofof200 °C◦(Table
200 4). 4).
C (Table
Temperatures of 200 °C or higher were not considered or confirmed through experiments. As a
Temperatures of 200 ◦ C or higher were not considered or confirmed through experiments. As a biomass,
biomass, SCG, which is a natural material, can suffer from carbonization or clogging due to
SCG, which is a natural material, can suffer from carbonization or clogging due to caramelization of
caramelization of residual saccharides. The compounding die was set in a circle shape with a
residual saccharides. The compounding die was set in a circle shape with a diameter of Φ 3 mm, to be
formed into the actual pellet. In the cooling process, a cooling line was installed by the air-cooling
type, and a cutting device capable of cutting the pellet to a certain size was connected at the end of
 Sustainability
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2019, 11,
11, xx FOR
FOR PEER
PEER REVIEW
REVIEW 55 of
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12
Sustainability 2019, 11, 1720 5 of 12
diameter of Φ 3 mm, to be formed into the actual pellet. In the cooling process, a cooling line was
installed by the air-cooling type, and a cutting device capable of cutting the pellet to a certain size
the cooling line (Figure 4). Conventional compounding processes are mostly water-cooled lines for
was connected at the end of the cooling line (Figure 4). Conventional compounding processes are
rapid cooling. However, in the case of SCG, because it is highly hygroscopic compared to a general
mostly water-cooled lines for rapid cooling. However, in the case of SCG, because it is highly
hydrophobic
hygroscopicplastic material,
compared it washydrophobic
to a general considered plastic
that it material,
would be it advantageous
was considered to block
that moisture,
it would be
so advantageous
the air-coolingtomethod was selected.
block moisture, so the air-cooling method was selected.

Figure3.3.Schematic
Figure Schematic of
of extrusion compoundingprocess.
extrusion compounding process.

Table 4. Experimental conditions of compounding pelletization process using extruder.

Table 4. Experimental conditions of compounding pelletization process using extruder.
Material
Material Spent Coffee
Spent Grounds
Coffee Grounds Polypropylene
Polypropylene
Material Spent Coffee Grounds Polypropylene
Mixing ratioratio
Mixing (%) (%) 0/10/20/30
0/10/20/30 100/90/80/70
100/90/80/70
Compatibilizer (phr)(phr)
Compatibilizer 33
Die diameter (φ) 3
Die diameter (Ф) 3
Motor RPM 1800
Motor
Screw RPM RPM 1800
120
Screw RPM 120
NZ H1 H2 H3 H4
Temperature (◦ C) NZ H1 H2 H3 H4
Temperature (°C) 200200 190190 180
180 160160 140 140

Figure 4. Processes of extrusion compounding experiments for pelletization: (A) Extruders, conveyors
and cutting machine for forming SCG-PP composite pellets. (B) Process for transferring extruded
molten SCG-PP composites using air-cooled conveyor belts. (C) Cutting process for pelletizing cooled
SCG-PP extruded strands.
 of SCG-PP composite pellets formed by varying the content of SCG based on the HOMO-PP and
BLOCK-PP matrix. The screw mounted on an injection molding machine (WOOJIN SELEX Corp.,
Product No. E-120) has an L/D of 28:1, and a clamping force of 120 tons. American Society for Testing
and Materials (ASTM) standard molds were used to measure mechanical properties. The temperature
of the process was controlled to 200 °C or less to prevent carbonization of SCG. The conditions of the
Sustainability 2019, 11, 1720 6 of 12
injection molding process are detailed in Table 5. Injection-molded specimens of Neat-PP and SCG-
PP composites are shown in Figure 6.
2.4. Injection Molding Process
Table 5. Experimental conditions of injection molding machine for confirmation of formability of
AnSCG-PP
injection molding
composite process (Figure 5) was carried out to evaluate the mechanical properties
pellets.
of SCG-PP composite pellets formed by varying the content of SCG based on the HOMO-PP and
Experimental Condition of Injection Molding Machine
BLOCK-PP matrix. The screw mounted on an injection molding machine (WOOJIN SELEX Corp.,
NZ H1 H2 H3 H4
Product No. E-120)Injection
has an L/Dtemp.of (°C)
28:1, and a clamping force of 120 tons. American Society for Testing
200 190 180 170 165
and Materials (ASTM) standard molds were used to measure mechanical
Injection press. (MPa) 5
properties. The temperature
of the process wasHolding
controlled to 200 ◦ C or less to prevent carbonization
press. (MPa) 3 of SCG. The conditions of the
injection molding process are detailed
Holding time (s) in Table 5. Injection-molded specimens
15 of Neat-PP and SCG-PP
composites are shown in Figure 6.
Cooling time (s) 30

Figure5.5.Schematic
Figure Schematicof
ofSCG-PP
SCG-PP composite
composite injection
injectionmolding
moldingspecimen
specimenpreparation.
preparation.

Table 5. Experimental conditions of injection molding machine for confirmation of formability of

SCG-PP composite pellets.

Experimental Condition of Injection Molding Machine

NZ H1 H2 H3 H4
Injection temp. (◦ C)
200 190 180 170 165
Injection press. (MPa) 5
Holding press. (MPa) 3
Holding time (s) 15
Cooling time (s) 30
Sustainability 2019, 11, x FOR PEER REVIEW 7 of 12

(A) (B)

Figure 6. ASTM standard injection molding specimens for measuring mechanical properties: (A) Neat
Figure 6. ASTM standard injection molding specimens for measuring mechanical properties: (A) Neat
HOMO-PP; (B) SCG30/PP70 composite.
HOMO-PP; (B) SCG30/PP70 composite.

2.5. Method of Measuring Mechanical Properties

Formability evaluation of SCG/PP composite pellets was carried out by ASTM specimens using
the injection molding process (Figure 6) and mechanical properties were measured. The impact
 Sustainability 2019, 11, x FOR PEER REVIEW 8 of 12

friendly materials for food containers and small household appliances that require impact resistance.
SCG decrease the crystallinity of HOMO-PP and increase the amorphous region, thereby minimizing
brittleness
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2019, 11,increasing
1720 the impact strength of HOMO-PP. 7 of 12
On the other hand, the impact strength of BLOCK-PP decreased by 39.7% as the SCG content
increased when the SCG content was 30%. The tendency of the reduced impact strength of BLOCK-
2.5.PPMethod of Measuring
is the same Mechanical
as in a previous study Properties
[17]. This is related to the copolymer type of BLOCK-PP. When
theFormability
content of SCG evaluation of SCG/PP strength
is low, the impact composite hardly decreases.
pellets However,
was carried out bysince
ASTM BLOCK-PP
specimens hasusing
a
low crystallinity compared to HOMO-PP, it is difficult to dramatically increase
the injection molding process (Figure 6) and mechanical properties were measured. The impact the amorphous region
by incorporating
strength (ASTM D256) SCG wasinto measured
BLOCK-PP,using and increasing the impact
a digital impact strength
tester of BLOCK-PP
(Salt Co. Ltd., Model is No.
expected
ST-120,
to be hard.
Incheon, Korea) and the tensile strength (ASTM D638) and flexural modulus (ASTM D790) were
The results of tensile strength measurements (Figure 8) indicated that tensile strength values
measured using UTM (Universal Testing Machine, QMESYS Co. Ltd., Model No. QM-100T, Seoul,
decreased when SCG was mixed with neat HOMO-PP and neat BLOCK-PP. These results are similar
Korea). Impact strength was measured in accordance with the ASTM D 256 method, and the specimen
to those of previous studies [19]. It is considered that the added SCG does not act as a reinforcing
sizes were 63.5 × 12.7 × 3.0 mm3 . The impact was applied to the side of the notch [28]. The tensile
material and acts as a micro-defect in the composites that reduces the tensile strength of the specimen.
strength was measured in accordance with the ASTM D 638 method, and the specimen sizes were
In addition, as the SCG increases content, phase separation with the matrix occurs and it is considered
165to×cause
19 ×a3.3 mm3 . in
decrease The cross-head
tensile strength speed
as anwas 10 mm/min
interface when [32].
defect occurs measuring the tensile strength [29].
The flexural modulus was measured in accordance with
The flexural modulus (Figure 9) also showed a tendency to decrease the ASTM D 790when
method,
SCGand
was the specimen
mixed and
sizes were the × 12.7 ×
127 highest 6.4 mm 3 . The support
showed value at 20%–30% of SCGdistance
content of specimens
among SCG/PP.wasHowever,
102.4 mm theand the test
flexural
load speed was
modulus of the10SCG/BLOCK-PP
mm/min [30]. The is notmechanical
significantly properties
different values were obtained
from Neat-PP by reduction
(only 1.5% averagingatthe
measured values of five specimens.
SCG30/BLOCK-PP compared to Neat-PP). Based on the results of the mechanical properties
measurement, the particles of SCG were not considered to act as a reinforcing agent, and acted as a
3. filler.
Results Theand Discussion
main constituents of SCG (g/100 g) are hemicellulose (36.7 g), mannose (21.2 g), galactose
(13.8
Forg),theprotein (13.6 of
evaluation g),the
andformability
glucose (8.6ofg)SCG-PP
[33]. Therefore,
compositeresidual
pellets,proteins in SCG may
the mechanical be the of
properties
reason
ASTM for decreased flexural
injection-molded modulus.
specimens were measured. Using HOMO-PP and BLOCK-PP as a matrix,
Figures 10 and 11 shows flexural
the content of SCG was increased to 10%, strength
20%, and and30%
Young’s modulus
by weight of SCG/PP.
to meet Flexural
the biomass strength
content of 25%.
decreased with the addition of SCG as flexural modulus. However, the Young’s modulus increased
The amount of MAPP added to improve compatibility between hydrophilic SCG and hydrophobic PP
with the addition of SCG. The increased Young’s modulus of SCG/PP is analyzed to be due to the
was 3 phr. MAPP is an additive that helps disperse SCG uniformly in the PP matrix, and it improves
intrinsic rigidity of SCG [19]. The higher the Young’s modulus, the more excellent the stiffness, so
the disadvantage of mechanical properties due to poor compatibility between plastic polymer resin
that this tendency can be applied to the manufacture of automotive interior materials which require
and the biomass SCG.
environment friendliness and high stiffness.
The results of the measurement (Figure 7) of the impact strength indicated that the mechanical
In addition, scanning electron microscope (JEOL Ltd., Product No. 7001F, Tokyo, Japan)
properties of thewere
observations composite pellets
performed based on the
to investigate the matrix HOMO-PP
morphology of the and
SCGBLOCK-PP
particles. Thewere opposite. This
cross-sectioned
result
test specimen for impact strength was frozen in liquefied nitrogen, fractured, and then measured. Itis a
is caused by the difference in structure between HOMO-PP and BLOCK-PP [31]. HOMO-PP
polymer polymerized
was confirmed with
that the SCGpropylene alone,
particles were so it haswith
combined highPP
regularity and crystallinity.
matrix (Figure On the
12). SCG is sieved other
with
hand,
a size of 300–600 µm, but since the SCG form clusters, the size of each individual SCG particle isthe
BLOCK-PP has lower crystallinity than HOMO-PP because of the ethylene polymerized into
arrangement
analyzed toof bepropylene.
smaller, such as 10–20 µm, which is similar to previous studies [17,18].

Figure
Figure 7. 7. Resultsofofimpact
Results impactstrength
strength measurement
measurement of
of composite
compositepellets
pelletsaccording
accordingtoto
the mixing
the ratios
mixing ratios
of SCG and
of SCG and PP. PP.

In the case of HOMO-PP, the impact strength increased as the content of SCG was increased;
the maximum value was increased by 52.8% when the SCG content was 30%. The increase in
impact strength of SCG/HOMO-PP was the first reported result, and is expected to be applicable
to eco-friendly materials for food containers and small household appliances that require impact
resistance. SCG decrease the crystallinity of HOMO-PP and increase the amorphous region, thereby
minimizing brittleness and increasing the impact strength of HOMO-PP.
Sustainability 2019, 11, 1720 8 of 12

On the other hand, the impact strength of BLOCK-PP decreased by 39.7% as the SCG content
increased when the SCG content was 30%. The tendency of the reduced impact strength of BLOCK-PP
is the same as in a previous study [17]. This is related to the copolymer type of BLOCK-PP. When the
content of SCG is low, the impact strength hardly decreases. However, since BLOCK-PP has a low
crystallinity compared to HOMO-PP, it is difficult to dramatically increase the amorphous region by
incorporating SCG into BLOCK-PP, and increasing the impact strength of BLOCK-PP is expected to
be hard.
The results of tensile strength measurements (Figure 8) indicated that tensile strength values
decreased when SCG was mixed with neat HOMO-PP and neat BLOCK-PP. These results are similar
to those of previous studies [19]. It is considered that the added SCG does not act as a reinforcing
material and acts as a micro-defect in the composites that reduces the tensile strength of the specimen.
In addition, as the SCG increases content, phase separation with the matrix occurs and it is considered
to Sustainability
cause a decrease
2019, 11, in tensile
x FOR PEER strength
REVIEW as an interface defect occurs [32]. 9 of 12

Sustainability 2019, 11, x FOR PEER REVIEW 9 of 12

Figure
Figure 8. 8. Resultsofoftensile
Results tensilestrength
strengthmeasurement
measurement of
of composite
compositepellets
pelletsaccording
accordingtoto
the mixing
the ratios
mixing ratios
of SCG and
of SCG and PP. PP.

The flexural modulus (Figure 9) also showed a tendency to decrease when SCG was mixed
and showed the highest value at 20–30% of SCG content among SCG/PP. However, the flexural
modulus of the SCG/BLOCK-PP is not significantly different from Neat-PP (only 1.5% reduction
at SCG30/BLOCK-PP compared to Neat-PP). Based on the results of the mechanical properties
measurement, the particles of SCG were not considered to act as a reinforcing agent, and acted as a
filler. The main constituents of SCG (g/100 g) are hemicellulose (36.7 g), mannose (21.2 g), galactose
(13.8 g),Figure
protein (13.6 g),
8. Results and glucose
of tensile strength(8.6 g) [33]. Therefore,
measurement residual
of composite pelletsproteins
accordingintoSCG may be
the mixing the reason
ratios
for decreased flexural
of SCG and PP. modulus.

Figure 9. Results of flexural modulus measurement of composite pellets according to the mixing ratios
of SCG and PP.

Figure
Figure 9. 9.Results
Resultsofofflexural
flexuralmodulus
modulus measurement
measurement of
ofcomposite
compositepellets
pelletsaccording
accordingtoto
thethe
mixing ratios
mixing ratios
of of
SCGSCG
andand PP.
PP.
Sustainability 2019, 11, 1720 9 of 12

Figures 10 and 11 shows flexural strength and Young’s modulus of SCG/PP. Flexural strength
decreased with the addition of SCG as flexural modulus. However, the Young’s modulus increased
with the addition of SCG. The increased Young’s modulus of SCG/PP is analyzed to be due to the
intrinsic rigidity of SCG [19]. The higher the Young’s modulus, the more excellent the stiffness, so
that this tendency
Figure 9. Resultscan be applied
of flexural to the
modulus manufacture
measurement of automotive
of composite pelletsinterior materials
according which
to the mixing require
ratios
environment
of SCG andfriendliness
PP. and high stiffness.

Figure
Figure 10. Results
Results of
of flexural
flexural strength
strength and
and Young’s
Young’s modulus
modulus measurement
measurement of composite
composite pellets
Sustainability
according
according2019,to11,
thex FOR PEER
mixing REVIEW
ratios of SCG and HOMO-PP.
HOMO-PP. 10 of 12

Figure
Figure 11. Results
Results of
of flexural
flexural strength
strength and
and Young’s
Young’s modulus
modulus measurement
measurement of composite
composite pellets
according
according to the mixing ratios of SCG and BLOCK-PP.
BLOCK-PP.

In addition, scanning electron microscope (JEOL Ltd., Product No. 7001F, Tokyo, Japan) observations
were performed to investigate the morphology of the SCG particles. The cross-sectioned test specimen
for impact strength was frozen in liquefied nitrogen, fractured, and then measured. It was confirmed
that the SCG particles were combined with PP matrix (Figure 12). SCG is sieved with a size of
300–600 µm, but since the SCG form clusters, the size of each individual SCG particle is analyzed to be
smaller, such as 10–20 µm, which is similar to previous studies [17,18].

Figure 12. SCG particles in PP matrix under mixed conditions of SCG30/PP70.

4. Conclusions
In this study, SCG/PP composite pellets were prepared through an extrusion compounding
 Figure2019,
Sustainability 11. 11,
Results
1720 of flexural strength and Young’s modulus measurement of composite pellets
10 of 12
according to the mixing ratios of SCG and BLOCK-PP.

Figure 12.
Figure 12. SCG particles in PP
PP matrix
matrix under
under mixed
mixed conditions
conditions of
of SCG30/PP70.
SCG30/PP70.

4. Conclusions
4. Conclusions
In
In this
this study,
study, SCG/PP composite pellets
SCG/PP composite pellets were
were prepared
prepared through
through an an extrusion
extrusion compounding
compounding
process
process toto explore
explore thethe material
material recycling
recycling method
method of of SCG,
SCG, aa waste
waste biomass,
biomass, andand to
to develop
develop sustainable
sustainable
environmentally friendly materials. ASTM standard injection-molded
environmentally friendly materials. ASTM standard injection-molded specimens were prepared forspecimens were prepared for
the evaluation of formability, and evaluation of mechanical properties was
the evaluation of formability, and evaluation of mechanical properties was performed. The extrusionperformed. The extrusion
compounding
compounding process process for
forthe
thecomposite
compositepellets
pelletsofof SCG-PP
SCG-PP and and
thethe injection
injection molding
molding process
process for
for the
the test specimens of mechanical properties were confirmed to have
test specimens of mechanical properties were confirmed to have good formability. SCG in compositegood formability. SCG in
composite
materials met materials met the standard
the standard for beingfor being a bio-based
a bio-based plastic, plastic, containing
containing up to 30%up toby 30% by weight.
weight. The
The measurement of mechanical properties showed that the mechanical property
measurement of mechanical properties showed that the mechanical property values were generally values were generally
lowered
lowered as the content
as the content ofof SCG
SCG increased.
increased. Since
Since the
the hydrophilic
hydrophilic SCG SCG and
and hydrophobic
hydrophobic PP PP are
are different
different
materials,
materials, itit is
is considered
consideredthat thatthe theinterfacial
interfacialadhesion
adhesionisispoor,
poor,andandisis considered
considered toto
bebe a key
a key factor
factor in
in lowering the mechanical properties due to phase separation. Therefore,
lowering the mechanical properties due to phase separation. Therefore, further research is being further research is being
conducted
conducted on on thethenecessary
necessarymodification
modificationofofthe thesurface
surface of of
SCG.SCG. However,
However, it was
it was confirmed
confirmed thatthat
the
the impact
impact strength
strength of neat
of neat HOMO-PP
HOMO-PP and and Young’s
Young’s modulus
modulus of PPofare
PPincreased
are increased
as theascontent
the content
of SCGof
SCG increased. These results can be applied to food containers, small
increased. These results can be applied to food containers, small household appliances, and household appliances, and
automotive interior products
automotive interior products requiring
requiring high
high impact
impact strength,
strength, highhigh stiffness,
stiffness, and
and environmentally
environmentally
friendly
friendly regulations. Disposable biomass, such as SCG, is glucose-based cellulose, soso
regulations. Disposable biomass, such as SCG, is glucose-based cellulose, it harmless
it is is harmless to
to
the human body and can be used as an environmentally friendly sensitive material. The SCG-PP
the human body and can be used as an environmentally friendly sensitive material. The SCG-PP
composite
composite material
materialpellet
pelletis is
expected
expected to be
to widely
be widely applicable to real-life
applicable applications
to real-life if it canifbeit applied
applications can be
to non-toxic products, such as disposable products and food
applied to non-toxic products, such as disposable products and food containers. containers.

Author Contributions: J.S.S. conceived and designed the experiments; C.-S.Y. and K.Z. performed the experiments;
Author Contributions: J.S.S. conceived and designed the experiments; C.Y. and K.Z. performed the experiments;
J.S.S. and Y.R. analyzed the data; S.W.C. funding acquisition; J.S.S. review and editing, J.S.S. wrote the paper.
J.S.S. and Y.R. analyzed the data; S.W.C. funding acquisition; J.S.S. review and editing, J.S.S. wrote the paper.
Funding: This research was supported by Basic Science Research Program through the National Research
Foundation of Korea (NRF) funded by the Ministry of Education (No. NRF-2018R1D1A1B07049405).
Acknowledgments: The first author would like to thank Sung Woon Cha for their advice and guidance.
Conflicts of Interest: The authors declare no conflicts of interest.

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