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Thermal Science and Engineering Progress

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Utilization of LDPE plastic waste on the quality of pyrolysis oil as an asphalt

solvent alternative
Dedy Hariadi a, Sofyan M. Saleh b, R. Anwar Yamin c, Sri Aprilia d, *
a
Doctoral School of Engineering Science, Universitas Syiah Kuala, Banda Aceh 23111, Indonesia
b
Civil Engineering, Engineering Faculty, Universitas Syiah Kuala, Banda Aceh 23123, Indonesia
c
Institute of Road Engineering (IRE) Ministry of Public Works Indonesia, Bandung, Indonesia
d
Chemical Engineering, Engineering Faculty, Universitas Syiah Kuala, Banda Aceh 23123 Indonesia

A R T I C L E I N F O A B S T R A C T

Keywords: Natural asphalt cannot be used directly because of hardness and low penetration, so it needs to be softened with a
LDPE plastic waste solvent. A solvent that can be used is from oil plastic pyrolysis as an alternative additive. Plastics are now an
Pyrolysis inseparable item from daily necessities and are the largest pollutant on the environment. Plastic is a polymer that
White plastics
is difficult to be decomposed, and one way to decompose it is through pyrolysis or thermal cracking. This
Mixed plastics
Blend plastics
research studies the quality effect of low-density polyethylene (LDPE) plastics waste on the quantity and quality
Quality effect of oil yield produced through the pyrolysis process in the three reactor outlets. LDPE plastics waste used was
distinguished: LDPE-White, LDPE Mixed-plastic, and LDPE Blend-plastic. The results showed that, in the process
of plastic pyrolysis LDPE, in addition to affecting the yield of produced oil, the quality of plastic is also influenced
by the length of time of pyrolysis. The better the quality of the plastic is, the higher the oil yield and the shorter
the pyrolysis times are. LDPE plastic pyrolysis at 250 ◦ C produces the maximum yield. Most oil yields, namely
99.78%, 75.60%, and 50.29% were produced by LDPE white plastics, mixed plastics, and blend plastics,
respectively, when pyrolyzed for 110, 180, and 270 min. The economic yields of each plastic of 88.78%, 60.68%,
and 40.35% were generated if each was hydrolyzed for 60, and 80 min.

1. Background
Asphalt is material that is dark brown to black, solid or semisolid,
consisting of natural components or obtained petroleum residue. On the
basis of the American Association of State Highway and Transportation
Office, the type of asphalt can be determined on the basis of the pene­
tration rates of the used asphalt. The greater the penetration value of the
asphalt is, the lower the level of asphalt hardness. Buton asphalt is
natural asphalt found in the Buton area, Southeast Sulawesi, Indonesia.
This asphalt contains bitumen and minerals that were mixed into a
single unit with a bitumen content of 15% to 30% and 70% to 85%
minerals [16]. Buton asphalt has high hardness (low penetration), so it
cannot be used directly. It is necessary to modify the asphalt as one
approach to improve performance. It is also necessary to add an additive
to soften the asphalt. Additives that can be added include light oil,
gasoline/naphtha, kerosene, diesel, or other diluents. One alternative as
a solvent is oil produced by the pyrolysis of plastic waste. The pyrolysis
product of plastic waste can be used as a softener in Buton asphalt and as
a binder in the asphalt mixture when aspen oil 60 is used [17]. For these
purposes, it is necessary to look for alternative solvents as additives,
especially products that are large-scale and economically cheap.
The use of plastic cannot be separated from daily life for industrial,
commercial, and household needs. Every year, the average person uses
700 plastic bags. Supermarkets globally provide more than 17 billion
plastic bags every year. Plastic can be used many times (reuse) and can
be recycled. However, most plastic ends up as rubbish. Plastic waste is
very difficult to naturally decompose and is currently the largest
pollutant on Earth.
Many types of plastic are used for industrial needs, and trade and
household needs such as polystyrene (PS), polypropylene (PP), poly­
ethylene terephthalate (PET), high-density polyethylene (HDPE), poly­
vinyl chloride (PVC), and low-density polyethylene (LDPE). LDPE is a
plastic with a density in the range of 0.91–0.94 g/mL; half of LPDE is
crystalline (50–60%) and has a melting point of around 115 ◦ C [2]. LDPE
plastic is flexible with an oily surface, strong, relatively translucent, and
very resistant to chemical compounds at temperatures below 60 ◦ C.

* Corresponding author.
E-mail address: sriaprilia@unsyiah.ac.id (S. Aprilia).

https://doi.org/10.1016/j.tsep.2021.100872
Received 19 July 2020; Received in revised form 27 January 2021; Accepted 4 February 2021
Available online 14 February 2021
2451-9049/© 2021 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
D. Hariadi et al.
Physically, LDPE has a smaller and more flexible molecular density
compared to that of HDPE. LDPE is widely used both as a plastic bag and
as food or beverage packaging. The advantages of LDPE as a packaging
material are the low price, easy manufacturing process, flexibility, and
being easily recycled [2]. According to Bell and Cave [3], the natural
decomposition of plastic waste by microorganisms takes 400–1000
years, having major negative impact on the environment [4,6].
Although in energy recovery through the plastic combustion process,
combustion can reduce the amount of plastic waste, it causes a new
problem in terms of the emissions generated in the form of the toxic
gases HCl, HCN, and NOx, which can interfere with health [5]. In this
case, the processing of plastic waste by feedstock/chemical recycling,
which produces products in the form of liquids, gases, and solids is
preferred and widely used. One feedstock recycling technology is py­
rolysis. At present, decomposition through plastics through the pyrolysis
process is expected to be an alternative in reducing environmental
pollution and as a solvent alternative to soft asphalt.
The study of plastic pyrolysis is carried out under different experi­
mental conditions, and with different reactor types, types of plastic
materials, pure or waste materials, with the aim of obtaining the optimal
content and quantity of liquid products. The temperature and time of
pyrolysis have a strong effect on the production of quality pyrolysis
processes. An experiment with mixed plastic in a batch reactor showed
that the maximal yield of the liquid phase was achieved at 477 ◦ C
[18,20]. Kaminsky and Zorriqueta [19] used a batch microreactor with a
volume of 100 mL, and at 400 ◦ C, more than 40% of the PP samples did
not react, while at 500 ◦ C, 98% of the samples passed the pyrolysis
process. At 500 ◦ C and 60 min in a fixed bed reactor, the mixed-plastic
waste pyrolysis achieved high quality and yield of the oil product [19].
However, according to Aguado et al. [1], the pyrolysis temperature at
which the chemical composition of plastic waste breaks and evaporates
is in the range of 500–800 ◦ C. According to Santo et al. [7], the plastic
pyrolysis process can be carried out in the temperature range of
100–400 ◦ C with a reaction time of 0–60 min, and the first drops
generally occur at temperatures around 120 ◦ C.
In this study, the pyrolysis process used a reactor that comprised
three outlets to separate gas, residue, and oil, shown in the scheme in
Fig. 1. The reactor could process input material and undergo chemical-
structure breakdown into a gas phase with or without residual solids
remaining. Expected produced pyrolysis products are gas, oil, and
charcoal [8]. Sumani and Any [9] studied which pyrolyzed LDPE plas­
tics produced oil, gas, and residue in the form of solids. The liquid
product that was evaporated contained tar and polyaromatic hydro­
carbons [1]. If perfect conditions are obtained, LDPE and HDPE plastic
pyrolysis can produce oil and gas without residue left, as achieved by
Aprian and Munawar [10].
Aprian and Munawar [10] studied pyrolysis temperature and time to
determine the quantity of produced output. According to them, the
highest yield of oil products in LDPE and HDPE plastics was when
Fig. 1. Scheme of pyrolysis process.
2
Thermal Science and Engineering Progress 23 (2021) 100872
pyrolyzed at 400 ◦ C with an operating time of 60 min. Meanwhile, ac­
cording to Sumani and Any [9], the optimal temperature of LDPE plastic
pyrolysis is around 550 ◦ C. Pyrolysis products are created in the form of
gases or liquids as a result of the main reaction rise as pyrolysis tem­
perature increases, while the remaining solids (residue) left in the retort
are reduced.
In addition, Lopez et al. [11] concluded in their study that, if the
classification of plastics and the separation of impurities are carried out
first on the plastic to be hydrolyzed, then 90% of the plastic is converted
into oil and gas. According to them, the composition of the raw material
(input) greatly affects the quality of the produced output. Al-Salem et al.
[12] similarly stated that plastic sorting based on grade or classification
is key to the success of plastic recycling, including through the pyrolysis
method. Mulyadi [13] found that the conversion of plastic waste into
fuel-quality liquid products showed prospective results to be developed.
On the other hand, controlling the conversion process is easier than the
incineration process is [14]. However, according to Scheirs [15], proper
plastic-waste conversion can produce a minimal yield of 40% of used
inputs.
This study aims to determine the effect of the quality of LDPE plastic
waste on the percentage of plastic oil produced from the pyrolysis pro­
cess based on temperature and time. The pyrolysis process used a reactor
with three outlets or products in order to obtain a light oil that can be
used as a solvent in Buton asphalt.
2. Research methods
This study elaborates LDPE plastics by pyrolysis noncatalysis in the
laboratory. The reactor used, as shown in Fig. 2, was a retort equipped
with a thermocouple and regulator to maintain stable operational tem­
perature. Retorts from these devices are 60 × 60 × 30 cm. The reactor
had three liquid outlets; 1, 2, and 3. The plastic used as input had three
variations in the quality of LDPE plastics, namely white LDPE plastics
(plastic-P): plastics derived from white colored plastic bags; mixed-
plastic LDPE (plastic-M) that comes from a mix of plastic bags of
various colors; and blended-plastic LDPE (plastic-B), which is LPDE
plastic which comes from both LDPE plastic bags and from other LDPE
bags such as sugar bags, warping plastics, and snack bags, containing
aluminum foil or not. Each used plastic is visually as shown in Fig. 3.
In this study, the plastic pyrolysis process was carried out at four
temperature variations, namely 150, 200, 225, and 250 ◦ C, and with
three variations in terms of input weight, namely 2000, 4000, and 6000
g. To optimize the contents of the retort before being pyrolyzed, the used
LDPE plastic waste was chopped in advance so that it was about 2 × 4
(cm) in size. Pyrolysis measurements were observed at 10 min intervals.
The time when results of the distillate first came out was considered as
the beginning of the pyrolysis process (t = 0). Pyrolysis was stopped if
Fig. 2. Pyrolysis reactor.
D. Hariadi et al. Thermal Science and Engineering Progress 23 (2021) 100872

Fig. 3. Typical Counts and Quality of LDPE Plastics.

the liquid did not drip again.

The resulting oil yield could be determined by weighing the liquid
(oil M-1, M-2, and M-3) produced at any given time interval. At the end
of pyrolysis, the solid (residue) left in the retort was weighed to deter­
mine its weight. The amount of gas wasted from the pyrolysis process is
known from the difference in the weight of the input with the total
weight of the oil yield and residue.

3. Results and discussion

The term used to refer to oil from reactor was determined on the
basis of the LDPE plastic category that was used as the input from which
outlet oil emerged. For example, oil (M) from the pyrolysis of white
LDPE (P) plastic that emerged from Outlets 1, 2, and 3 is referred to as
MP-1, MP-2, and MP-3, respectively; for LDPE (M) mixed-plastic py­
rolysis oil, it was termed as MM-1, MM-2, and MM3; and blended-plastic
LDPE (B) as MB1, MB-2, and MB-3. Total oil from outputs 1, 2, and 3 is Fig. 5. Oil-yield effect of initial weight and temperature pyrolysis for LDPE
Plastic-M.
referred to as Total Oil (TM).

3.1. Oil yield of plastic pyrolysis effect of temperature

The effect of temperature and plastic types on pyrolysis product

yields, especially on liquid oils, are shown in Figs. 4–6. All types of
plastic waste that were degraded into liquid oil starting at 150–250 ◦ C
were investigated in the reactor that had three outlets. Fig. 4 shows that
the Plastic-P pyrolysis process carried out at 150 ◦ C did not produce any
oil at all (zero yield) either at inputs of 6000 or 4000 and 2000 g. At this
temperature, the pyrolysis process only converted most (90%) inputs
into residues, and the remainder into gas. The oil yield output of MP-1,
MP-2, and MP-3 oil was only produced at pyrolysis temperatures of
around 200 ◦ C, with the first drop occurring at the temperature range of
160–190 ◦ C. The temperature of the first drop was different from that

Fig. 6. Oil-yield effect of initial weight and temperature pyrolysis for LDPE
Plastic-B.

delivered by Santo et al. [7], which was around 120 ◦ C. This was due to
differences in the type of used plastic, the temperature at which the
pyrolysis process takes place, where Santo et al. [7] pyrolyzed plastics
from beverage bottles at 400 ◦ C.
The oil yield of TM-P was not produced even though the temperature
was increased. This condition applied to all given feeds. However, high
oil yield was produced on the use of a maximal input of 6000 g, which
was hydrolyzed at 250 ◦ C, which was equal to 99.89% and consisted of
13.85% MP-1, 32.49% MP-2, and 53.56% MP-3, with no residual solids.
Fig. 5 shows that the Plastic-M pyrolysis process carried out at 150 ◦ C
only produced TM-M yields of 3.36% and 3.92% MM-3, respectively, for
inputs weighing 2000 and 4000 g. For the 6000 g input, temperature
pyrolysis did not produce any oil yield at all. In the pyrolysis process
carried out at 150 ◦ C, 78.51% of 2000 g of input became residue, and the
remainder was converted into gas (18.13%). For 4000 g of input,
Fig. 4. Oil-yield effect of initial weight and temperature pyrolysis for Plastic-P.

3
D. Hariadi et al. Thermal Science and Engineering Progress 23 (2021) 100872

43.21% became residue, and 52.87% became gas. This shows that LDPE
mixed-plastic pyrolysis was very inefficient when performed at 150 ◦ C.
At temperatures above 200 ◦ C, the pyrolysis of plastic-M at all var­
iations in the weight of inputs used in this study could produce TM-M
yields, with first drops occurring in the range of 170–195 ◦ C. Howev­
er, the highest TM-M was only produced at 250 ◦ C. In the plastic-M
pyrolysis process at temperature as mentioned above (250 ◦ C), the use
of inputs weighing 2000 g produced as much as 90.08% (1801.55 g) TM-
M and 6.34% residual solids. At this temperature, if the input was
increased to 4000 g, the required time for the pyrolysis process increased
to 210 min, but the yield of TM-M was decreased to 68.51% (2740.3 g)
and residual solids increased to 13.04%. In the 6000 g input, 75.60%
(4535.8 g) became TM-M without leaving any residual solids when
hydrolyzed for 180 min. Thus, the LDPE mixed-plastic pyrolysis process
produces TM-M when performed using an input of at most 6000 g at
250 ◦ C. Fig. 8. Oil-yield effect of initial weight and temperature pyrolysis for LDPE
Fig. 6 shows the oil yield of Plastic-B pyrolysis. At 150 ◦ C, all vari­ Plastic-M.
ations in the input weight of used Plastic-B could produce oil from all its
outlets, namely MB-1, MB-2, and MB-3, respectively. Fig. 6 shows that
the resulting yield remained in line with the temperature rise. In addi­
tion to temperature, output yield was in line with the number of used
inputs.
There were differences between three variations of plastic type: in
Plastic-P (white plastic), oil cannot be produced at 150 ◦ C, but for
Plastic-M and Plastic-B at this temperature, the production of oil occurs.
This condition is different from that of Plastic-P pyrolysis, which only
produces oil at 200 ◦ C. On the other hand, for Plastic-M pyrolysis at a
temperature of 150 ◦ C, only Outlet 3 produced oil (MM-3). This showed
that the quality of Plastics-B was different and below the quality of
Plastics-M, and especially against the quality of Plastics-P. As with the
results of Plastic-P and Plastic-M pyrolysis, the highest yield of Plastic-B
pyrolysis results for all variations of input weight also occurred at
250 ◦ C. For all temperature variations, the highest yield was produced
with the 6000 g input. Oil yield was at a high percentage for Plastic-P,
followed by Plastic-M and Plastic-B.
Fig. 9. Oil-yield effect of initial weight and temperature pyrolysis for LDPE
Plastic-B.
3.2. Oil yield of plastic pyrolysis effect of time

Figs. 7–9 show the amount of oil produced from a pyrolysis process
determined by length-of-time pyrolysis. This experiment concerned an
initial mass of plastic waste of 6000 g. At the basis of the mass at 6000 g,
oil yield was found for all types of the plastic effect of temperature. Fig. 7
shows the oil yield from Plastic-P. The relationship between the maximal
yield of TM output produced by the length of time of the pyrolysis
process was calculated from the first drop of oil produced to the last drop
measured during the Plastic-P pyrolysis process.
Fig. 7 shows that the fastest TM-P yield rate occurred in the first 30
min from the first produced drop. After that and until 30 min, the second
TM-P rendement speed that occurred slightly decreased; after more than
Fig. 7. Oil-yield effect of initial weight and pyrolysis time for LDPE Plastic-P.
60 min since the first produced drop, the yield of produced TM-P
experienced a sharp decrease; lastly, after the 100th relative minute,
there was no subsequent increase (no further increase in total quantity
even though the length of the pyrolysis process was extended, which
indicated that the pyrolysis process was complete). This tendency
occurred in the TM-P yield, and to that of MP-1, MP-2, and MP-3. The
white LDPE plastic pyrolysis process was, therefore, economical when
performed with an input weighing 6000 g at 250 ◦ C for 60 min. The
white LDPE plastic pyrolysis process under these conditions produced a
total oil yield of 88.78%, which consisted of 12.662% MP-1 yield,
27.85% MP-2, and 48.32% MP-3 yield.
Fig. 8 shows the relationship of the maximal yield of TM-M output
produced by the length of time of the pyrolysis process, calculated from
the first produced oil drop until the last drop. This figure shows that,
even though the input pyrolysis process was 6000 g of the LDPE plastic
mix, 250 ◦ C for 180 min produced the most oil, which the oil yield was
75.60% and consisting of yields MM-1, MM-2, and MM-3 of 11.57%,
30.82%, and 33.21%, respectively. When compared with the percentage
of total oil plus gas yield obtained from this study (75.60% + 24.40%)
compared to that obtained by Lopez et al. [11], resulting in pyrolysis at
500 ◦ C during 30 min on plastic packaging and other packaging mate­
rials, which was 90%.
Plastic-M pyrolysis for 180 min produced the highest oil yield.
However, time duration is not necessarily an economical duration,
because the highest yield of TM-M (49.97%) was produced in the first
30 min since the first drop was produced. In the minute 70, the quantity
was increased to 63.21%; after that, there was only a small increase in
yield. Thus, the LDPE mixed-plastic pyrolysis process is economical

4
D. Hariadi et al. Thermal Science and Engineering Progress 23 (2021) 100872

when performed with as much as 6000 g at 250 ◦ C for 60 min. LDPE

mixed-plastic pyrolysis under these conditions produced a total oil yield
of 63.21%, consisting of a 9.81% yield for MM-1, 25.92% for MM-2, and
27.47% for MM-3.
Fig. 9 shows the oil yield of pyrolysis process at 6000 g mass of
Plastic-B with the effect of time. In Plastic-B, in 90 min from the first
drop of yield, there was an increase in TM-B yield of 34.01%, from
6.34% to 40.35%. In the extension of time until the pyrolysis process
was completed (minute 270) for another 180 min, there was an increase
in total oil yield of only 9.94%. Thus, 6000 g of LDPE-plastic blend at
250 ◦ C produced a maximal TM-B yield of 50.29% (consisting of yields
MB-1, MB-2, and MB-3 of 10.56%, 21.74%, and 17.99%) with a pyrol­
ysis duration of 270 min. However, the LDPE blended-plastic pyrolysis
process is economical if carried out for 90 min. At that duration, the
generated yield of TM-B was 40.35%, consisting of yields MB-1, MB-2,
and MB-3 of 9.75%, 16.75%, and 13.85%, respectively.
The condition of LDPE blended-plastic pyrolysis obtained from the
results of this study was different from that carried out by Aprian and
Munawar [10]. With a reactor with a diameter of 20 cm and a height of Fig. 11. Change in color of pyrolysis oil of LDPE Plastic-M.
40 cm, and by using 500 g of chopped (1–2 cm) LDPE plastic waste
(blend plastics), they obtained the maximal pyrolysis conditions at
400 ◦ C for 60 min. This difference may be due to differences in the
configuration and size of the pyrolysis reactor and the quantity of used
inputs.
The time of pyrolysis for all types of plastic waste affected the per­
centage of oil yielded. Plastic-P gave the highest oil yield from Plastic-M
and Plastic-B at the same feed to the reactor at 6000 g. Oil yield was
higher at Output 3 for all types of plastic waste.

3.3. Color change for pyrolysis oil

Oil color from the pyrolysis process was obtained from collecting oil
at the initial time until 120 min. Figs. 10–12 show that the color of the
oil pyrolysis production was different depending on the temperature
pyrolysis and type of plastics. By increasing the pyrolysis temperature,
the produced oil was darker. Fig. 10 shows the visualization of white
plastic (Plastic-P). On Plastic-P, discoloration is clearly visible; with
increasing temperature, the color changed from light yellow, to yellow,
to dark yellow. At 200 ◦ C, the oil was light yellow; at 225 ◦ C, it was
yellow; and at 250 ◦ C, the oil was dark yellow for MP-1, MP2, and MP3.
Fig. 12. Change in color pyrolysis oil of LDPE Plastic-B.
Fig. 11 shows the visualization of oil obtained from LDPE Plastic-M
(MM-1, MM-2, and MM-3). Three types of plastic were mixed, and the
color was darker than that of the white plastic (Plastic-P). At 200 ◦ C, The visualization of oil obtained from the LDPE Plastic-B (MM-1,
MM-1 was still dark yellow, and MM-2 changed a little into dark yellow MM-2, and MM-3) is shown in Fig. 12. The blended plastic gave the dark
at 225 OC. At 250 ◦ C, Plastic-M (MM-3) was black. color for all plastic blends because all plastics were blended without
separating impurities in the plastic waste.

4. Conclusions

In the process of plastic pyrolysis LDPE, the quality of the plastic

greatly influences the produced yield of plastic oil. For white LDPE
plastics, the pyrolysis process that produced the highest total oil yield
(99.89%) consisted of 13.85% MP-1, 32.49% MP-2, and 53.56% MP-3,
and occurred for 6000 g at 250 ◦ C for 110 min. However, it is
economical if performed for 60 min, with total oil yield results of
88.78% (12,621% MP-1, 27.85% MP-2, and 48.32% MP-3). For white
LDPE mixed plastics, the pyrolysis process that produced the highest
total oil yield occurred when using an input of 6000 g at 250 ◦ C for 180
min. Under these conditions, a total oil yield of 75.60% consisted of MM-
1, MM-2, and MM-3 yields of 11.57%, 30.82%, and 33.21%. The
economical condition occurred when it was hydrolyzed for only 70 min
with a total oil yield of 63.21% (9.81% MM-1; 25.92% MM-2 and
27.47%). For LDPE blended plastics, the pyrolysis process that produced
the highest total oil yield (50.295%) took place using an input of 6000 g
at 250 ◦ C for 270 min. However, it was economical if performed for 80
Fig. 10. Change in color of pyrolysis oil of LDPE Plastic-P.

5
D. Hariadi et al.
min, with a total oil yield of 40.35%, which consisted of 9.75% MB-1,
16.75% MB-2, and 13.85% MB-3. In the LDPE plastic pyrolysis pro­
cess, the difference in the quality of the plastic, in addition to affecting
the produced oil yield, also affected the temperature and length of time
of the process. Liquid oil from plastic waste pyrolysis contains impurities
such as sulfur, chlorine, solid residue, moisture, and acids. The presence
of these impurities both decreases the liquid quality of oil and limits its
asphalt application.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgments
The authors would like to thank the collaboration between the De­
partments of Civil Engineering and Chemical Engineering of Universitas
Syiah Kuala, and the Institute of Road Engineering (IRE) of the Ministry
of Public Works of Indonesia for the facilities provided to conduct the
experiment in the present work.
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