Pyrolysis of polypropylene waste with

natural zeolite as catalyst

Cite as: AIP Conference Proceedings 2114, 050019 (2019); https://doi.org/10.1063/1.5112463
Published Online: 26 June 2019

Emi Erawati, Hamid, and Resti Dian Permatasari

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AIP Conference Proceedings 2114, 050019 (2019); https://doi.org/10.1063/1.5112463 2114, 050019

© 2019 Author(s).
Pyrolysis of Polypropylene Waste with Natural Zeolite as
Catalyst
Emi Erawati1,a), Hamid1 and Resti Dian Permatasari1
1
Chemical Engineering Department, Engineering Faculty,
Universitas Muhammadiyah Surakarta. Jl. A.Yani Tromol Pos I, Pabelan, Kartasura, Surakarta, Indonesia
57102
a)
Corresponding author: emi.erawati@ums.ac.id

Abstract. Putri Cempo Landfill located in Surakarta, Central Java, Indonesia is one of landfills that have not been
equipped with appropriate waste management. Scavengers will sort out the garbage and collect it to garbage
collectors. Bottle cap was used as the sample of pyrolysis of polypropylene. Our research investigated various
temperatures and ratios of raw material to catalyst variation and standard diesel fuel. One hundred grams of caps
was inputted to the reactor. Temperature was controlled by thermocouple with variation of temperature of 400, 410,
420, and 430ºC. Every 20 minutes, bio-oil as the liquid product was collected to the storage. Noncondensable gas
was stored in three gallons. The amount of water flow from the gallons was assumed as the volume of the gas. Gas
pressure was controlled by open manometer while temperature by thermocouple. Every 20 minutes, the mass of the
gas was measured. Solid residue was measured after 120 minutes. At the temperatures of 430ºC and 410ºC, the
highest liquid yields and the highest gas yield were obtained, of 55.74% and 49.10%, respectively. From the ratios
of raw material to catalyst of 66:33; 75:23; 80:20; and 83:17 wt%, the highest liquid yield of 72.17% was identified
in the ratio of 66:33% wt% while the highest gas yield was 36.43. Our research found no residue solid. The
dominant chemical component was C13H28O. Bio-oil was analyzed with specification, such as specific gravity, API
gravity, gross heating value, flash point, pour point, and kinematic viscosity and found that it is feasible as diesel
fuel based on the Decree of the Directorate General of Oil and Gas of 2008.

INTRODUCTION

Based on the total number of residents, Surakarta is the third biggest city in Java, Indonesia, after
Bandung and Malang. Moreover, the total number of residents of Surakarta increases from 503,421 people
in 2010 to 514,171 in 2016.[1] Similar to other typical big cities, Surakarta has been developing many
sectors, such as industry, services, housing, education, transportation and so on. In the tourism sector, the
Local Government of Surakarta has provided permits for the establishment of new hotels since 2010. In
2018, a total of 52 hotels are available in Surakarta City. A number of national and international events have
been scheduled in Surakarta City, leading to an increase in hotel occupancy rate. Yet there is an adverse
impact of the increasing number of tourists in Surakarta City, which is an increase in the total of garbage or
municipal solid waste or trash.[2] TPA Putri Cempo is the landfill where all garbage is piled up with the
process of open dumping. Nevertheless, this open dumping method is not feasible to be applied in the future.
Furthermore, municipal waste are divided into three categories, namely organic fraction that can be
composted, combustible fraction mainly composed of paper and plastic, and non-combustible fraction of
mineral and metals.[3] The waste-related problems caused by an increase in population requires an
appropriate waste management.[4] Based on the data of the waste produced in Surakarta City, the produced
wastes can be classified into food waste, paper, cardboard and nappies, garden waste and wood, rubber and

Exploring Resources, Process and Design for Sustainable Urban Development

AIP Conf. Proc. 2114, 050019-1–050019-9; https://doi.org/10.1063/1.5112463
Published by AIP Publishing. 978-0-7354-1850-9/$30.00

050019-1
leather, plastic, metal and glass. The amount of garbage produced in Surakarta City in 2008-2017 (10 years)
is specified in Fig. 1.

150,000,000

Tranported Garbage
100,000,000
50,000,000

(kg)
0

2008
2009
2010
2011
2012
2013
2014
2015
2016
2017
Year

FIGURE 1. The garbage produced in Surakarta City in 2008-2017

(Source: The Environmental Services of Surakarta).

Figure 1 Shows that in 2008 to 2017, the amount of total garbage increases from 80,493 ton/year to
106,278 ton/year. If the percentage of plastics waste is assumed 10% of the total garbage, there were 8,049.3
ton/year and 10,627.8 ton/year of plastic waste in 2008 and 2017, respectively. Meanwhile, the global
municipal solid waste is expected to increase into 2.2 billion ton/year by 2025[4], in which the USA
contributes 254 million tons (12.8% of them is plastics [5], Western Australia contributes 750,000 tons
household waste [6], Bangkok contributes 8,291 to 11,500 tons/day [7], India contributes 127,486 tons/day
or 1.5-2.5 million tons/year [8], and Europe contributes 25.8 million tons municipal solid waste.[9] Similar
problem is also endured by Surakarta City whose municipal solid waste/MSW has not been managed
appropriately.
The landfill site in Surakarta City is called TPA Putri Cempo. Open dumping is employed for
managing organic waste. Nevertheless, organic waste undergoes continuous degradation of biodegradable
components under anaerobic condition, resulting in the production of biogas consisting of CH4 and CO2.[10]
Consequently, when rainfall occurs, the precipitation will drop on the organic waste and form leachate. The
composition of leachate contains of organic matter, heavy metal, and inorganic salt.[11] In the Putri Cempo
landfill, organic waste is processed into methane gas, while leaf waste is processed into compost. Moreover,
it is common that the landfill is used by the local community to herd livestock.
Despite of the existing waste management, the plastic waste transported into Putri Cempo landfill has
not been optimally processed. Plastic waste is collected to garbage collectors. Basically, plastic waste can be
processed through pyrolysis, gasification and combustion processes. The differences between the processes
can be seen in Table 1.[12]
TABLE 1 The differences between pyrolysis, gasification, and combustion process
No. Gasification Pyrolysis Incineration
1. Principle Partial Thermal degradation Full oxidative combustion
oxidation of organic material
Absence of oxygen
2. Operating 800-1,600 400-800 850-1,200
temperature
(ºC)
3. Reaction Ash and slag Ash and char Solid
product
4. Pre treatment Required Required Not necessary
5. Raw MSW Usually not Usually not Usually preferred
preferred preferred

The advantages of pyrolysis process include the simple design equipment, unnecessary waste sorting-
out, minimum environmental impact, utilization of all waste materials into different bio-products, and
syngas can be used in different energy applications, such as engines, boilers, fuel cell, turbine, and heat
pump.[13] Gasification process can convert solid and liquid hydrocarbon feedstock into synthetic gas that is
suitable for electricity production or manufacture of chemicals, hydrogen, or transportation fuels. There are
two disadvantages of gasification process. Firstly, air separation to obtain oxygen is more complex and

050019-2
costly. Secondly gasification uses air in which the nitrogen remains as an inert component in the producer
gas and dilutes the fuel gas leading to lower caloric value of fuel.[14] Moreover, the impact of incineration
will cause greenhouse gas emissions (GHG-E). However, the process can reduce the amount of specific
emissions, for example, sulphur dioxide, hydrogen fluoride, nitrogen oxide, total organic carbon, hydrogen
chloride, carbon monoxide, dust, and volatile heavy metal.[13]
Several researchers have studied pyrolysis of polypropylene (PP) using catalysts, such as
mesoporous silica MCM-41 and Al MCM-41[15], the mixing of polyethylene and polypropylene using
USY[9], the mixing of polyethylene and polypropylene using HZSM-5, USY, NH4ZSM-5, BHZSM-5,
BUSY, BHN4ZSM-5, and acid leachete[16], the mixing of polypropylene and Laminaria japonica using
zeolite[17], K2CO3 and ZnCl2[18], natural zeolite[19] , the mixing of polypropylene and oil shale[20], the
mixing of polypropylene and high density polyethylene[21], vegetable oil mixed with polypropylene[22],
zinger natta [23], the mixing of polyethylene and polypropylene[24], polypropylene and coffee waste[25],
without catalyst [26, 27, 28], ratio between Co and Al2O3, Co and CeO2, combination between Co, Al2O3,
CeO2[29], and waste and virgin polypropylene.[30]
The aims of our research are to investigate the influence of the temperature rate and raw material to
natural zeolite (wt%) on gas, liquid, and solid yields in the pyrolysis of polypropylene waste, to identify the
physical properties of fuel, namely its specific gravity, API gravity, gross heating value, flash point, pour
point, kinematic viscosity, and to identify chemical composition of pyrolysis of polypropylene waste.

MATERIAL AND METHOD

Plastic bottles are considered as polypropylene (pp). raw materials were bought from waste collectors
around the tirtonadi bus station, surakarta, central java, indonesia. natural zeolite as the catalyst was bought
from bratachem. the bottle caps as the source of pp are demonstrated in Fig. 2 and equipment used in the
research can be seen in Fig. 3.

FIGURE 2. Caps as the source of PP waste. FIGURE 3. The Pyrolysis Equipment.

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 The pyrolysis equipment consisted of a reactor with a capacity of two kilograms, diameter of 25 cm,
and height of 40 cm, a condenser, two thermocouples, two liquid storages, a manometer, and three gas
storages. Liquid petroleum gas was used for the combustion process. two thermocouples were installed to
monitor the process, one in the pyrolysis chamber (reactor) and the other at the exit line of the condenser. the
raw materials were cleaned up and cut into an even size of 3x3 cm. approximately 1,000 grams of bottle
caps was put into the reactor that was connected to a thermocouple in order to control the temperature. the
pipe at the top of the reactor was connected to a cyclone which separates gas from solid. gas produced by the
reaction was condensed using the first condenser, resulting in a liquid product that was then collected. the
produced gas which was not condensed was re-processed in the second condenser and the yield was stored
in three gallons. the gas volume was calculated based on the volume of water flowing from the gallon. the
process was repeated with various ratios of plastics to natural zeolite, namely: 67:33 wt%; 75:25 wt%; 80:20
wt%; and 83:17 wt%. pyrolysis was performed for two hours, and the sample was weighed every 20 minutes
to measure the changes in mass of the gas and liquid. after 120 minutes, the solid sample was examined to
determine the mass of final solid.[31] the other properties were analyzed with astm method [32].

RESULTS AND DISCUSSION

The change in mass of bio-oil, gas, and solid

As shown in Fig. 4(a), the relationship between the liquid mass and temperature variation is presented.
At 410ºC, from beginning or the starting condition to the first twenty minutes, the mass degraded very
slowly. After twenty minutes, degradation rapidly increased. However, after two hours, the total liquid mass
was relatively stable at approximately 500 grams. Meanwhile, in various catalyst rates, no liquid was gained
from the initial condition to the first twenty minutes. After one hour, the decomposition of liquid began to
advance much faster as demonstrated in Fig. 4(b).

600.00 1000.00
Mass of Liquid (g)

Mas of Liquid (g)

Temperature of Raw Material

400.00 400ºC :Catalyst =
500.00
200.00 Temperature of 66:33%w/w
0.00 410ºC 0.00 Raw material :
-80 20 120 -80 20 120 catalyst =
Temperature of
Time (minutes) 75:25%w/w
Time (minutes) 420ºC

(a) (b)
FIGURE 4. The change of liquid pyrolysis profile (grams) over time (minutes) with variation of: (a) temperature, and
(b) ratio of raw material to catalyst.

The changes in mass of gas over time and the ratio of raw material and catalyst are shown in Fig. 5(a)
and (b). The production of gas started after a third of an hour. the total mass of gas at two temperatures
variants (420 and 430ºc) was five higher than at 400ºc. Meanwhile, the four variations of the ratio of plastics
to natural zeolite catalyst were 67:33 wt%; 77:23 wt%; 80:20 wt%, and 83:17 wt%. Fig. 5(b) shows the mass
of gas in the ratio of plastic waste to the catalyst of 66:33 wt%, which was identified as the highest.

050019-4
 400.00 200.00 Raw material :

Mass of Gas (g)

Mass of Gas (g)

200.00 Temperature of 100.00 Catalyst =66 :
400ºC 33 %w/w
0.00 0.00
0 20406080100120 Temperature of 0 20 40 60 80100120 Raw material :
410ºC Catalyst =77 :
Time (minutes) Time (minutes)
23 %w/w

(a) (b)
FIGURE 5. The change in mass of gas (grams) over time (minutes) with variation of: (a) temperature, and (b) ratio of
raw material to catalyst.

Figure 6 a and 6b illustrate the changes of residual solid over time based on temperature and the ratio
of raw material.
1000.00 1000.00
Raw
Mass of Solid (g)

Mass of Solid (g)

800.00 Temperature of 800.00
material :
600.00 400C 600.00 Catalyst = 67
400.00 400.00 : 33 %w/w
Temperature of
200.00 410C 200.00
Raw
0.00 0.00
Temperature of material :
0 20 40 60 80100120140 020
46080100
0120 Catalyst = 77
430C
Time (minutes) Time (minutes)
: 33%w/w

(a) (b)
FIGURE 6. The change in mass of residual solid (grams) over time (minutes) with variation of temperature and the
ratio of raw material to the catalyst.

The Product of Pyrolysis of Polypropylene

The products of pyrolysis of polypropylene are relatively different among studies, including oil and
wax[19], bio oil, bio-char and non-condensable gas [33, 9, 34, 35], and solid residue and tar[28]. In the
present study, the products of pyrolysis are bio oil and gas.
The vertical bar chart (Fig. 7) illustrates the relationship between the yields of liquid, gas, and solid
and temperature variations. There are four temperature variations, namely 400, 410, 420 and 430ºC. The
lowest liquid yield was 49.10% that was obtained at 410ºC. The proportions of liquid yield at temperatures
of 400, 420 and 430ºC were 51.48%, 53.23%, and 55.74%, respectively. A study on waste and original
polypropylene[30] reported the result of the yield of gas, liquid, and solid of 11%, 76% and 13% (virgin
polypropylene) compared to 15%, 71% and 14% (waste polypropylene), respectively.

60.00 51.48 50.90 53.23 55.74 80.00 72.17 69.01 71.86 63.57
50.00 48.52 49.10 44.26
46.77
60.00
Yield (%)

40.00
36.43
30.00 40.00 27.83 30.99 28.14
Yield (%)

Liquid Liquid
20.00 Yield 20.00 Yield
10.00
Gas Yield 0.00 Gas
0.00
200 250 333 500 Yield
400 410 420 430
Temperature ( ºC) Mass of Zeolite (g)

FIGURE 7. The relationship between temperature variation FIGURE 8. The relationship between the variation of
and yield. mass of catalyst and yield.

050019-5
 The vertical bar chart (Fig. 8) describes the relationship of the composition of zeolite and raw material
with liquid and gas yields. there were four variations given in the ratio of raw material to natural zeolite,
namely 66:33 wt%, 75:25 wt%, 80:20 wt%, and 83:17 wt%. The experiments found that the higher the rate
of zeolite to raw material, the lower the liquid yield. The highest percentage of liquid yield was 72.17%,
which was obtained by the ratio of 66:33 wt%. The percentages of liquid yield at the other three variants
were 69.01, 71.86, and 63.57%, respectively. It indicates that at the rates of raw material to natural zeolite of
66:34 wt% and 80:20 wt% are relatively stable at approximately 27.99%. From our research and [36], it can
be claimed that when the mass of catalyst is increased, the yield of liquid is reduced. Nevertheless, in these
variations, there was no solid residue resulting from the process.

Composition of the Product of Pyrolysis

Bio-oil as liquid product was also analyzed by using gas chromatography with mass spectrometry
(GCMS). Our research found there were four dominant chemical compositions, namely isotrydecanal, 2-
heptenal, 1-heksadecanesulvonyl chloride, 1-hexadecanol 3,711,15-tetramethyl. The percentage of chemical
composition can be seen in the Table 2.

TABLE 2 The Chemical Composition of Bio-Oil

Chemicals Area (%) Molecular Formula

Isotridecanal 32.94 C13H28O

2-heptenal 10.38 C13H28O
1-Heksadecanesulvonyl 8.53 C13H28O
chloride
1-hexadecanol 3,7,11,15- 9.91 C13H28O
tetramethyl

Some researchers have conducted studies on pyrolysis of polypropylene and different chemical
compositions are obtained. Some of them are olefins, aromatics, furan, pyran, aliphatic oxigenates[16],
benzene, ethyl benzene, naphthalene, phenol, xylene, toluene[10], toluene, ethyl benzene, xylene, alkyl
benzene C10 and C11[16], acid, oxygenates, other hydrocarbons, monoaromatic hydrocarbon, polyaromatic
hydrocarbon, and phenolic[17], alkenes and olefins [36], 2-methyl-1-pentene, 3-methylcyclopentene, 1-
heptene, 1-octene, C4-C13 hydrocarbon, over C14 hydrocarbon, benzene, toluene, xylene, ethylbenzene,
indene, biphenyl, benzene, ethyl benzene, naphthalene, phenol, xylene, and toluene, toluene, xylene,
dimethyl-benzene, methyl styrene, trimethylbenzene, propenyl benzene, naphthalene.[30]. Meanwhile, the
dominant chemical composition in our research was C13H28O.

Liquid products from various temperatures and ratio of natural zeolite compositions were analyzed.
the liquid analysis result can be seen in Table 3, which shows that according to data analysis, the liquid
product is solar (diesel) fuel that is feasible based on the decree of the directorate general of oil and gas,
ministry of energy and mineral resources of the republic indonesia, no. 14496k/14/djm/2008 concerning the
standards and quality (specifications) of oil fuels of the combustible oil variety traded in indonesia. the
liquid products were found to have similarities to diesel fuel in terms of the value, specific gravity, gross
heating value, pour point, and kinematic viscosity.

050019-6
 TABLE 3 The analysis of bio-oil with variations in temperature and ratios of raw material to natural zeolite
Indonesian Zeolite
N Temperatur
Characteristics Unity National Composition [29] [30] [39]
o. e Variation
Standard Variation
1 Specific Gravity - 0.742 0.7740 0.7673 0.7932 0.77 0.86
. at 60/60°F
2 API Gravity - - 51.3 52.9 46.47 33.0
. 3
3 Gross Heating MJ/kg ൒41.87 46.65 46.74 41.86 40.8
. Value
4 Flash Point PM °C min 60 <20 <18 40 30
. c.c
5 Pour Point °C Max. 18 -18 - 12 <10 -9
.
6 Kinematic mm2/s 2.0-5.0 1.324 1.167 2.149 2 4.09
. Viscosity at
40°C

CONCLUSION

From the research, the following points can be concluded:

1. At higher temperature, the bio-oil yield increases while the gas yield decreases.
2. In the variation of the ratio of raw materials to catalyst, the higher the catalysts, the lower the yield of bio-
oil and the higher the yield of gas.
3. Based on experiments with various temperatures and ratios of the catalyst to the raw material, no residual
solids are obtained.
4. The liquid product has been found to be feasible as diesel fuel based on the Decree of the Directorate
General of Oil and Gas of 2008.

ACKNOWLEDGEMENTS

The authors would like to express their utmost gratitude for the financial sponsorship from the
Ministry of Research, Technology, and Higher Education of the Republic Indonesia through the Applied
Product Grand Scheme, Contract Number: 211.27/A.3-III/LPPM/V/2017.

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