International Journal of Environmental Science and Technology (2022) 19:4019–4036

https://doi.org/10.1007/s13762-021-03381-4

ORIGINAL PAPER

Fuel production by thermal and catalytic co‑pyrolysis of polyethylene

terephthalate and polyethylene using waste iron as catalyst
S. Malik1 · H. Gulab1 · K. Hussain1 · M. Hussain2 · M. A. Haleem1

Received: 13 October 2020 / Revised: 17 March 2021 / Accepted: 7 May 2021 / Published online: 22 May 2021
© Islamic Azad University (IAU) 2021

Abstract
Waste low-density polyethylene (LDPE), high-density polyethylene (HDPE) and polyethylene terephthalate (PET) were co-
pyrolyzed thermally and catalytically using waste iron dust (Fe) as a catalyst in a close-packed steel batch reactor. Various
reaction conditions like temperature, reaction time, mixing ratio, catalyst proportion and initial mass of the reactants were
optimized for effective conversion of the waste plastics. Outcomes of the thermal and catalytic reactions were compared to
evaluate the catalytic activity of waste Fe in terms of oil yield and total percent conversion. The product oils were fraction-
ated in gasoline, kerosene and diesel ranges. The physicochemical properties of the samples fractions were found to be in
close resemblance with the physicochemical properties of the standard fuels. The FTIR analysis indicates aromatic, satu-
rated and unsaturated hydrocarbons in all the samples and alcoholic OH in the Fe-catalyzed reaction product. The GC–MS
analyses confirmed the saturated, unsaturated and aromatic hydrocarbons in various fractions ranging from lighter to heavier
hydrocarbons in accordance with their boiling point distribution. The catalytic oils were found to contain relatively lighter
hydrocarbons as compared to the non-catalytic oils. Calorific values of the catalytic oil and fractionated samples were found
to be higher than the corresponding standard fuels.

Keywords  Co-pyrolysis · LDPE · HDPE · PET · Hydrocarbons

Introduction chemicals in the form of gas or liquid (Manos et al. 2001).

A huge amount of the plastics waste in the environment is
of great concern regarding its management and harmful
effects. Although the conventional methods of waste plastic
disposal, i.e., dumping in landfills and incineration, absorb
a large amount, they produce toxic compounds. The recy-
cling process in which the waste thermoplastics are melted
and remolded into other products also has limitations due to
low-quality products (Aguado et al. 2007; Jan et al. 2010a,
b). Recently, the novel method of treating the waste plastics
is the thermal or catalytic degradation (Adil et al. 2007).
The products of degradation process can be used as fuel and
Editorial responsibility: Agnieszka Galuszka.
* H. Gulab
hussaingulab@gmail.com
1
Department of Chemistry, Bacha Khan University
Charsadda, Charsadda, KPK, Pakistan
2
Department of Physics, Bacha Khan University Charsadda,
Charsadda, KPK, Pakistan
The thermal process usually employs a high temperature and
gives a broad range of hydrocarbons. The catalytic process
on the other hand produces selective products with higher
yields relatively at lower temperature making the process
cost-effective (Guohua et al. 2000; Jan et al. 2013). In this
way, waste plastics can serve as a cheap energy source. The
use of catalysts has several advantages, e.g., lowering the
reaction temperature, production of fuel range hydrocarbon
in a single step and eliminating the requirement of upgrada-
tion of fuel (George et al. 2000). Different plastics have been
tried to be degraded by using different catalytic and pho-
tocatalytic processes (Miandad et al. 2019; Antelava et al.
2020; Haq et al. 2020; Sana et al. 2020, Ilyas 2019). Vari-
ous studies reveal that the degradation processes have been
catalyzed using metals as catalyst. The copper metal has
been used for co-pyrolysis of coal and polypropylene, and
the iron metal has been found effective in the co-pyrolysis
of biomass and polyethylene (Hussain et al. 2016; Gulab
et al. 2016). Similarly, aluminum and copper have been
employed in the pyrolysis of biomass (Gulab et al. 2019), as
the polyethylene terephthalate (PET) is converted into wax

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4020 International Journal of Environmental Science and Technology (2022) 19:4019–4036
as a result of catalytic and non-catalytic pyrolysis and can-
not be converted into liquid product separately. Therefore,
in the present study, the most common waste plastics, i.e.,
low-density polyethylene (LDPE), high-density polyethylene
(HDPE) and polyethylene terephthalate (PET), have been
co-pyrolyzed using waste iron dust (Fe) as catalyst with the
intention to develop methods for their proper disposal, clean
the environment and recover a renewable energy resource.
Another aim of the present study is to convert PET into use-
ful liquid product instead of wax with the help of co-pyroly-
sis in combination with other waste plastics and Fe catalyst.
Materials and methods
Collection and preparation of waste plastics
Waste bottles made of HDPE (with identification code 2),
PET (with identification code 1) and waste plastic bags made
of LDPE were collected from the household wastes. The
samples were washed with detergent and sun-dried. Then,
these were cut into small pieces of about 1.36–9.92 ­mm2 size
and stored for further use.
Preparation of catalyst
The waste iron dust was collected from the blacksmith’s
workshop produced as a result of grinding iron for various
purposes. The iron dust was passed through a mesh size 40
corresponding to a 0.42-mm particle size, which was then
directly used as a catalyst.
Fig. 1  Experimental setup for
pyrolysis, 1. electric furnace,
2. reactor, 3. temperature
controller, 4. thermocouple, 5.
condenser, 6. stand, 7. collect-
ing flask, 8. ice bath, 9. outlet
for non-condensable gases
13
Pyrolysis reactor
The waste plastic was pyrolyzed in an indigenously designed
batch steel reactor. The reactor was consisted of two cylin-
drical portions, i.e., the lower portion and upper portion
(lid). The lid had a 10.6-cm delivery tube with 1.1 mm inter-
nal diameter that was quick fitted on the lower portion. The
reactor’s height was 14 cm with 6 cm internal diameter. The
lid and lower portion were provided with curved ridges for
prevent mixing of the products and reacting materials. The
reactor’s volume was 395.8 c­ m3. The reactor was placed
inside a locally made electrical furnace equipped with a
resistance coil, thermocouple and temperature controller.
The furnace worked on 220 V AC and provided a heating
rate of 0.5 °C S­ −1. The schematic diagram of pyrolysis pro-
cess is shown in Fig. 1.
Procedure
Various reactions were carried out under different reaction
conditions for the optimization study. The catalytic activity
of the Fe catalyst was examined by comparison of the cata-
lytic reactions with the non-catalytic reactions. Reactions
were carried out in triplicate in order to obtain reproducible
results. In order to carry out a catalytic reaction, a known
amount of the catalyst and waste plastic or mixture of waste
plastics were added to the pre-weighed reactor. The reactor
was sealed and made air tight by means of Teflon. The deliv-
ery tube of reactor was connected with the condenser lead-
ing to the collection flask. The condenser and the collection
flask were also pre-weighed. The pre-weighed reactor was
placed in the furnace, which was then turned on. The tem-
perature was set in the range 400–500 °C. The temperature
International Journal of Environmental Science and Technology (2022) 19:4019–4036 4021

was increased with a heating rate of 0.5 °C ­S−1 up to the final
set temperature. The temperature was kept constant at final
temperature for a fixed time, e.g., 30, 60, 90 or 120 min. On
completion of pyrolysis reaction, the reactor was removed
and cooled down to room temperature in order to weigh the
reaction products. During the reaction, four types of prod-
ucts were formed, i.e., oil, wax, gases and coke. Oil and wax
were collected in the collection flask, while some wax was
left in the upper lid of the rector as well as in the condenser.
The condensable gases were condensed into liquid, and the
non-condensable gases were expelled out. The quantities
of oil, wax and coke were calculated from the pre-weighed
and post-weighed reactors. The amount of non-condensable
gases was calculated from the known quantities as under;
Wt. of non − condensable gases = Reactants−(oil + wax + coke)
The percent weight of the oil, wax, coke and gases was
calculated using the following formulas:
Oil wt.
%wt.of oil =
Raw plastic wt.
× 100
Wax wt.
%wt.of wax =
Raw plastic wt.
× 100
Total% conversion = %wt.of oil + %wt.of wax + %wt.of gases
(6)
Measurement of physicochemical parameters
of the liquid product
Various physicochemical parameters and fuel properties of
the product oil were determined according to the standard
ASTM methods. Viscosity of the sample oils was deter-
mined using viscometer. Specific gravity was found by the
ASTM-D1298 method, while API gravity was calculated
from the specific gravity. Flash point was determined by
Rapid Tester, Model RT-1, Erdco Eng. Corp. Pour point,
cloud point and aniline point were determined accord-
(1) ing to ASTM-D97, ASTM-D2500 and ASTM-D611-82
methods, respectively. ASTM distillation was carried out
employing ASTM-D86-16a method. Similarly fractional
distillation was also carried out by means of fractionating
column. Refractive index was measured by Palm Abbe
(2) Digital Refractometer model; PA202, MISCO, USA. The
calorific value of oil was determined using Bomb Calorim-
eter model; AC500, Leco Corporation, USA.
(3)

FTIR analyses
Coke wt.
%wt.of coke =
Raw plastic wt.
× 100 (4)
The FTIR analyses were carried out using FTIR Spectrum
2, PerkinElmer, USA. The scanning was performed from
gases wt. 4000 to 450 ­cm−1 at a resolution of 4 ­cm−1.
%wt.of gases = × 100 (5)
Raw plastic wt.

Fig. 2  Effect of process tem-

94.8

100
perature (20% PET, 40% LDPE,
91

90

40% HDPE, time: 60 min, non- 90 Oil

catalytic)
80
75.3

80 Wax

70 Gases
60.3
59.3

Coke
% Conversion

60
Total % Conversion
50
40.7

39.7

40
32.3
24.7

24.7
21.4

30
13.2

20
17.3

20
11.5

10
3.2

9
5.2

10
0
6

5
3
2

0
0

0
400 425 450 475 500 525
Temperature (°C )

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4022 International Journal of Environmental Science and Technology (2022) 19:4019–4036

GC–MS analyses temperature was 300 °C, while the detector temperature

The oil samples were analyzed using GC–MS, Clarus
SQ-8, PerkinElmer, USA. Helium was used as carrier
gas at a pressure of 70.1 kPa. The capillary column with
5% phenyl methyl siloxane as stationary phase, 0.25 mm
diameter, 0.25 um phase thickness and 30 m length was
used with a constant gas flow of 1 mL ­min−1. The injection
was also held at 300 °C. The split ratio was 20. The oven
temperature programming was varied from sample to sam-
ple as required.
The MS was set at EI + ionization mode while recording
the m/z from minimum to the maximum. The chromatogram
peaks were identified using MS library, NIST 2014, version
2.4.

Fig. 3  Effect of reaction time 90

85
84
(20% PET, 40% LDPE, 40%

80
HDPE, non-catalytic) 80

70
54.5
60
% Conversion

50.7
Oil
45.5

45.4
50
39.7 Wax
40
32.3

Gases
30

25.6
30
Coke

20
20
15.5

15.7
20
16

15
13

10
8
0

0
30 60 90 120
Time (min)

Fig. 4  Pyrolysis of indi- 110

96.7

vidual PET, LDPE, and HDPE

95.9

(reactants mass: 10 g, Temp.: 100

87.9

500 °C, Time: 60 min, non-

90
catalytic)
80
69.6
67.2
% Conversion

70 Oil
52.7

60 Wax
43.2

50 Gases
Coke
40
27.1

Total % Conversion
30
20.7

12.1

20
4.1

10
3.3
0

0
PET LDPE HDPE

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International Journal of Environmental Science and Technology (2022) 19:4019–4036 4023

Results and discussion in the temperature caused to increase the gases production,

Optimization of process conditions
Effect of process temperature
The effect of temperature on the co-pyrolysis of PET (20%),
LDPE (40%) and HDPE (40%) has been investigated from
400 to 525 °C. It can be seen from Fig. 2 that in the tempera-
ture range of 400–450 °C, most of the reactants remained
intact and amount of the residue is higher. Therefore, fur-
ther reactions were carried out at higher temperature. At
500 °C, the total % conversion of the reactants was found up
to 80% during the non-catalytic process. A further increase
which was not desirable. Thus, a 500 °C was selected as
workable temperature for the co-pyrolysis under the given
conditions. A similar pattern in the gas formation has been
noticed by Demirbas (2004) using a temperature range of
277–627 °C for a mixture of polypropylene, polyethylene
and polystyrene. The gas yield was found to increase from
12.3 to 42.4%, while the oil yield was increased with tem-
perature till 477 °C and then decreased till 627 °C.
Reaction time
The non-catalytic co-pyrolysis process was carried out for
the mixed plastics with the same ratio at 30, 60, 90 and

Fig. 5  Effect of polymers ratio 110

98
(Temp.: 500 °C, reactants

89.8
92.1
100

93

83.5
mass: 10 g, time: 60 min, non-
catalytic)
90

68.7
80 Oil
% Conversion

56.1
70
56.2

55.7

39.7
46.6
43.2
41.8

60 Wax
36.9

38.1

43.8
30.6
50 36.4

31.3
40 Gases
2

16.5
30

10.2
20
7.9
0

10
0

0
0

P= PET, L=LDPE, H=HDPE

Fig. 6  Pyrolysis of individual
94.5

100
PET, LDPE, and HDPE (reac-
88.9
86.8

tants mass: 20 g, temp.: 500 °C, 90

time: 60 min, non-catalytic)
80

70
58.6
56.7
% Conversion

Oil
60
50.9

Wax
50
Gases
35.9

40 Coke
29.5
27.2

30 Total % Conversion
13.2

20
11.1

6.4

5.5

10
5
0

0
PET LDPE HDPE

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4024 International Journal of Environmental Science and Technology (2022) 19:4019–4036

120 min reaction time while taking 20 g starting material at
500 °C. It was observed that the reactants were converted up
to 80% in a 60-min reaction time (Fig. 3). A further increase
up to 90 and 120 min caused increase in the total % conver-
sion up to 84% and 85%, respectively. However, keeping in
view cost-effectiveness of the process, longer than 60-min
reaction time cannot be recommended as increase in the
product was not considerable. Thus to achieve the promis-
ing results in terms of maximum reaction products within
the limited reaction time, application of a suitable catalyst
was required. Consequently, the iron dust (Fe) obtained from
the wastes was applied as catalyst for this purpose, where the
reaction time was kept constant at 60 min. The influence of
reaction time was also investigated for 10 g of initial mass
of the mixture of PET (20%), LDPE (40%) and HDPE (40%)
at 500 °C for 60 min non-catalytically. It was observed that
keeping the reaction conditions same, the total % conver-
sion was around 93% for the reaction carried out with 10 g
initial reactants mass. Thus, 60 min can be used as optimum
time for the completion of reaction using 10 g initial mass
of the reactants. However, with 10 g initial mass, the oil
yield approaches 0% in cases of both the non-catalytic and
catalytic reactions. If the initial mass of the raw material is
further increased, i.e., 40 g and 80 g, the total % conversion
would be lesser as compared to 10 g and 20 g initial mass in
the 60-min reactions. Thus, if the initial mass is increased,

Fig. 7  Effect of polymers 90
ratio (temp.: 500 °C, reactants

80

76.4
78
80

71.3
mass: 20 g, time: 60 min, non-

74

73
catalytic)
70
Oil
60
% Conversion

42.7
39.7 Wax

40

43.4
50
38 22

28.7 27.9
30.3
32.3

Gases
36.4
35.5

26 34
40
34

Coke

27
30 23.6
Total % Conversion
20

20
4.5
8

10
6

0
0

P= PET, L=LDPE, H=HDPE

Fig. 8  Effect of catalyst/ 100%

polymer ratio (20% PET, 40%
86

LDPE, 40% HDPE, Temp.: 90%

81.2

84
85

500 °C, Reactants mass: 20 g,

80

Time: 60 min) 80%

70%
% Conversion

53.1

60% Oil
50.7

49.8

50% Wax
40.2
39.7

Gases
32.3

40%
25.4

Coke
30%
20.5
21

19.2
18.8

Total % Conversion
20

15.6

13.3

16
12.4

20%
15
15

14

10%
8

0%
0.0% 2.5% 5.0% 7.5% 10.0%
Catalyst % amount

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International Journal of Environmental Science and Technology (2022) 19:4019–4036 4025

the reaction time may be increased accordingly in order to
achieve the required % conversion. This means that using a
reactor having a specific volume, the optimum reaction time
will be different for different initial masses of the reactants.
Lopez (2011) has reported that a 30-min reaction time is
optimum for the total conversion of mixture of plastics in
a fixed bed reactor of 3.5 mL volume. In another autoclave
reactor having 300 mL volume, the reaction time has been
reported to be 60 min for a mixture of various plastics at
500 °C (William and Slaney 2007).
Effect of reactants initial mass
All the three waste plastics, i.e., PET, LDPE and HDPE,
were taken individually as reactants and pyrolyzed at 500 °C
for 60 min, but no liquid products were produced where the
initial mass of the reactant was kept as 10 g (Fig. 4). It was
also observed that taking 10 g initial mass of the reactants,
i.e., PET, LDPE and HDPE, with a percent ratio of 20, 40
and 40, respectively, produced no liquid product both cata-
lytically and non-catalytically at 500 °C in a 60-min reaction
time (Fig. 5). However, when the initial mass was doubled,
i.e., 20 g, the oil was formed in both the cases of individ-
ual plastic and mixture of all the three plastics as shown in
Figs. 6 and 7, respectively. This could be attributed to the
high pressure developed within the reactor due to enhanced
production of gases at the fixed reactor’s volume as a result
of increased mass of the reactants.
The advantage of taking small quantity of the reactants
is that relatively a higher total percent conversion can be
achieved in a 60-min time as the heat transfer could be effec-
tive within the smaller mass, but higher frequency of the
batch reactions and reproducibility of the results could be
disadvantages of the process in this case. Reason for the non
reproducible results could be that the composition of reac-
tants is not uniform as the reactant waste plastics are made
by different companies with different organic dyes and color
additives. Further, the waste plastics stay for longer time in
the environment after being used by the consumers; they
possibly adsorb other impurities as well (Miskolczi et al.
2013). All these factors affect the process and final products
of the pyrolysis.

Table 1  Physicochemical Fuel properties Co-pyrolytic* Co-pyrolytic* Parent oil Pyrolytic Parent Pyrolytic
properties of the co-pyrolytic Parent oil catalyzed by Fe oil of LDPE Parent oil of
and pyrolytic oil HDPE

Refractive index 1.4358 1.4372 1.431 1.436

Specific gravity 0.858 0.744 0.780 0.782
API gravity 33.42 58.69 49.91 48.75
Flash point (°C) 12.00 12.00 12.00 13.00
Pour point (°C) 23.00 8.00 5.00 − 13.00
Cloud point (°C) 25.00 12.50 7.00 − 5.00
Aniline point (°C) 59.00 52.00 54.00 56.50
Calorific value (cal/g) 10,721 12,680 10,987 10,967

*LDPE (40%), HDPE (40%), PET(20%)

Table 2  Physicochemical properties of catalytic oil fractions in gasoline, kerosene and diesel ranges in comparison with the standard fuels
Fuel properties Fraction in gasoline Fraction in kerosene Fraction in Diesel Standard ­valuesa
range (30–180 °C) range (160–230 °C) range (200–320 °C)
Gasoline Kerosene Diesel

Refractive index 1.4333 1.4541 1.4583 1.4340 1.4423 1.4637

Specific gravity 0.731 0.810 0.850 0.72–0.78 0.77–0.82 0.81–0.89
API gravity 62.07 43.19 34.97 70–52 40–52 39–35
Flash point (°C) 8.0 8.0 10.0 − 43  > 38 74
Pour point (°C)  < − 40.0 − 11.0 16.0 – − 18 −7
Cloud point (°C) − 13.0 − 6.0 18.0 – – –
Aniline point (°C) 59.0 61.0 72.0 – – –
Calorific value (cal/g) 11,882 11,205 11,213 10,246–10,915 10,311–11,052 10,246–11,225
a
 Petroleum Product Surveys. http://​www.​afdc.​energy.​gov; Fuel properties http://​webse​rver.​dmt.​upm; Games GS (2015), Herbert and Donnell
(1977), Boniphace (2018), Jan (2010a, b)

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4026 International Journal of Environmental Science and Technology (2022) 19:4019–4036

Effect of polymers ratio
Effect of different proportions of PET, LDPE and HDPE
was investigated by degrading all the three plastics in dif-
ferent ratios under the same process conditions. All the
three waste plastics were also pyrolyzed separately under
similar conditions. As already mentioned under “Effect of
reactants initial mass” section, that no liquid product was
obtained while taking 10 g initial mass of the waste plastic
in the isolated reaction, similar results were obtained while
taking all the three plastics with cumulative initial mass
of 10 g, both catalytically and non-catalytically during
the co-pyrolysis under the optimized reaction conditions.
Therefore, a 20 g of the starting material with different
proportions of PET, LDPE and HDPE was used for the
co-pyrolysis. It can be seen from Fig. 6 that the LDPE and
HDPE separately produced 88.9% and 94.5% oil, respec-
tively, in the non-catalytic reactions at 500 °C in 60 min,
while the PET produced no oil both catalytically and non-
catalytically at the optimized reaction conditions.
During the co-pyrolysis, it was observed that maximum
oil was produced at a mixing percent ratio of 20:40:40 of
PET, LDPE and HDPE, respectively (Fig. 7). The results
show that in combination with LDPE and HDPE, the PET
acted as a retardant in oil production. The optimized ratio
of PET was found to be 20%, where oil was produced in
combination with the LDPE and HDPE. Thus, components
of a mixture of plastics affect the product yield as reported

Fig. 9  ASTM distillation curves Non-catalytic Oil Fe catalyzed Oil

for the catalytic and non-cata-
lytic oil 400

350

300
Temperature (°C)

250

200

150

100

50

0
10 20 30 40 50 60 70 80 90 100
Volume of distilled Oil (mL)

Fig. 10  FTIR spectra of the

catalytic and non-catalytic oil

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International Journal of Environmental Science and Technology (2022) 19:4019–4036 4027

Table 3  Composition of the S/N. Retention time (min) Hydrocarbons Wt%

parent catalytic oil
1 2.26 4-Acetyl-1-methylcyclohexene 0.40
2 2.45 2,4-Dimethyl-1-heptene 1.10
3 2.50 2-Nonene 1.00
4 2.77 1,7-Heptanediol 0.30
5 3.06 2-Methyl-2-oxiranyl cyclobutanone 1.10
6 3.11 1-Decene 4.72
7 3.17 4-Methyl octane 6.96
8 3.45 9-(3-furanyl)-2,6-dimethyl-2,6-Nonadien-4-one 0.40
9 3.90 3,7-Dimethyl-1-octene 6.63
10 3.93 2,3-Dimethyl-octane 4.32
11 3.97 Decane 1.91
12 4.01 3,5-Dimethyl- octane 0.90
13 4.17 4-Tetradecene 4.32
14 4.25 5-Tetradecene 1.20
15 4.67 Bicyclo (2,2,1) 2-butylheptane 1.51
16 4.73 3-Dodecene 7.03
17 4.80 2-Methylnonane 5.22
18 4.95 Oxalic acid, isobutyl nonyl ester 0.60
19 5.48 4-Methyl-2,7-octadiene 1.51
20 5.54 1,12-Tridecadiene 7.33
21 5.60 1-Tridecene 5.42
22 5.80 1-Undecene 0.90
23 6.07 9-Oxabicyclo nonane 0.50
24 6.26 1-Eicosyne 1.41
25 6.32 6-Dodecene 6.73
26 6.37 2,6-Dimethyl undecane 3.92
27 6.62 Bicyclo-8-methylene-octane 0.20
28 6.73 3,8-Nonadien-2-one 0.80
29 6.97 1-Hexadecanol 1.81
30 7.04 2-Propenoic acid, tridecyl ester 5.52
31 7.09 2-Butyl-1-octanol 3.11
32 7.22 Cyclohexane, 1,1-dodecylidenebis-4-methyl 0.60
33 7.72 5-Tetradecene 7.13
34 7.77 2-Methyl-8-propyl dodecane 1.91
35 7.90 3-Butyl cyclohexanone 0.70
36 7.98 2,6,8-Trimethyl decane 0.50
37 8.36 2,3,6,7-tetramethyl octane 0.80
38 8.41 2,3-Dimethyldecane 0.90
39 8.71 Carbonic acid, methyl tridecyl ester 0.40
40 8.98 1-Heptacosanol 1.41
41 9.01 9-hexyl heptadecane 1.00
42 9.42 2-methyl-1-Butanol 0.30
43 9.62 5,8-diethyl dodecane 0.50

in a study where during the co-pyrolysis of PE and PS,
increase in mass of the PS in mixture caused to increase
the liquid yield and degradation rate (Lee 2012).
The purity and contamination of the waste plastics
have also an impact on the product yield and its qual-
ity. Studies have revealed that the waste plastic is always
contaminated; therefore, the pyrolysis products and pro-
cess are greatly affected. Williams et  al. reported that
under the same reaction conditions, when pure and waste
plastics were pyrolized, the pure plastics mixture and
waste plastics mixture yielded the liquid product as 48.7%
and 32.5%, respectively (Hussain et al. 2016).

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4028 International Journal of Environmental Science and Technology (2022) 19:4019–4036

Fig. 11  Chromatogram of the parent catalytic oil

Fig. 12  Chromatogram of the non-catalytic parent oil

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International Journal of Environmental Science and Technology (2022) 19:4019–4036 4029

Table 4  Composition of the S/No. Retention time (min) Hydrocarbons Wt%

parent non-catalytic oil
1 5.4 5-Ethyldecane 4.56
2 6 2,6,10,14-Tetramethyl heptadecane 3.45
3 6.29 2,8,10,14-Tetramethyl heptadecane 0.99
4 6.44 Tetracontane-3,5,24-trimethyl 2.46
5 6.69 Ethylene 0.37
6 8.05 4-Dodecen 5.54
7 8.20 4-Propyl heptanes 3.94
8 9.80 6-Dodecene 7.39
9 9.94 2,6,7-Trimethyl decane 7.27
10 10.27 2,4,10,14-Tetramethyl heptadecane 5.17
11 11.47 6-Tridecene 6.40
12 11.60 7-Tetradecene 5.79
13 12.89 2-Methyl 4-Nonene 5.30
14 13.01 2,6-Dimethyl heptadecane 6.65
15 13.17 3-Methyl tridecane 3.69
16 14.54 9-Tetradecene 3.08
17 14.65 5-Methyl tetradecane 2.59
18 14.92 Hexadecen 3.69
19 15.14 2,4,7-Trimethyl decane 1.85
20 15.95 6-Tridecene 1.85
21 16.58 4,4-Dimethyl-non-5-enal 0.99
22 16.69 15-Heptadecenal 3.08
23 16.79 Decane, 2,6,8-trimethyl 2.83
24 17.28 Cyclohexadecane 0.99
25 17.37 2,4-Dimethyl heptadecane 0.86
26 18.22 3-Dodecene 1.48
27 18.30 4-Methyl tridecane 1.97
28 18.75 2,6,10,15-Tetramethyl heptadecane 1.60
29 19.55 Hexadecen-1-ol 0.99
30 19.63 9-Octyl heptadecane 1.23
31 20.72 7-Hexyl eicosane 0.25
32 20.77 2-Methyl-7-hexadecene 0.25
33 20.84 2,6,6-Trimethyl decane 1.23
34 2.97 2-Methyl heptadecane 0.25

Effect of catalyst
In order to investigate the effect of Fe catalyst, different reac-
tions were carried out at the optimized non-catalytic reaction
conditions where the weight of catalyst was varied as 2.5%,
5.0%, 7.5% and 10.0% of the weight of reactants (Fig. 8). It
can be observed from the results that with increasing ratio
of the catalyst from 2.50 to 5.0%, the oil, gases and total %
conversion have been increased, while the yield of wax and
coke has been decreased, which is obviously intended. At
a ratio of 7.5%, the catalyst has not caused any increase in
the product yields except a negligible increase in the gases.
It is also noteworthy that with a further increase in the ratio
of catalyst up to 10.0%, the conversion has been relatively
decreased. The reason could be trapping of the oil product
within the increased mass of catalyst for a fixed time of reac-
tion. Similar results have been observed in another study
where increasing the amount of Y-zeolite catalyst beyond
11% has a negative effect on polymer conversion (Gulab
et al. 2010). Thus, 5.0% catalyst to reactant ratio was consid-
ered as optimum, which was used for further studies. Many
authors have found different optimum values for various
catalysts, e.g., Gaurh and Pramanik (2013) used two types
of ZSM-5 catalysts for a mixture of plastics with optimum
plastic-to-catalyst ratio of 20:1 and 30:1 at 600 °C. Abbas
Abadi et al. found that a catalyst-to-polymer ratio of 20 wt%
was optimum for the maximum conversion of HDPE into
liquid oil (Abbas et al. 2014).

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4030
Fig. 13  Chromatogram of the catalytic oil fraction obtained in the Gasoline range
Physicochemical properties of the liquid product
The physicochemical properties of the parent catalytic and
non-catalytic oil obtained from the co-pyrolysis of LDPE,
HDPE and PET were studied and compared with pyrolytic
oil obtained from LDPE and HDPE separately as well as
with the standard fuel values (Table 1).
The physicochemical properties of the distillation frac-
tions of the catalytic parent oil and their comparison with the
standard fuel values are also presented in Table 2.
It could be seen from the results that the distillation frac-
tions are having physicochemical properties resembled to
that of the standard fuels gasoline, kerosene and diesel.
However, based on the physicochemical properties, the par-
ent oil may be further fractionated in order to improve its
quality in terms of matching with the standard fuels.
ASTM distillation
Both the catalytic and non-catalytic oils were distilled
using ASTM distillation method, and the obtained curves
are given in Fig. 9. It can be seen from the figure that over
the whole range of distillation, the catalytic oil has been
distilled relatively at a corresponding lower temperature
than the non-catalytic oil. Obviously, the reason could
13
International Journal of Environmental Science and Technology (2022) 19:4019–4036
be formation of lighter hydrocarbons due to the catalytic
activity of waste Fe catalyst during the catalytic degrada-
tion process. The curve for catalytic oil shows that about
55% of the oil has been distilled in the gasoline range (up
to 180 °C), 25% oil has been distilled in the kerosene range
(180–250 °C) and 20% oil has been distilled in the diesel
range (250–300 °C) as described by Willium and Gary
(2011). The non-catalytic oil curve shows that around
28% oil covers the gasoline range, 20% oil matches the
kerosene range and 20% oil is in the diesel range, while
the rest of 32% fraction is composed of further heavier
hydrocarbons. The maximum distillation temperature for
the catalytic oil was found to be 300 °C, while for non-
catalytic oil it was 350 °C. The ASTM distillation results
for the catalytic oil are in close agreement with its frac-
tional distillation results, where 62.5%, 16.6% and 12.5%
oil were distilled in gasoline, kerosene and diesel ranges,
respectively. Around 4.1% wax was obtained and 4.3%
oil was converted into gases due to further cracking of
hydrocarbons during the ASTM distillation.
FTIR analysis
The oil obtained from the co-pyrolysis of LDPE (40%),
HDPE (40%) and PET (20%) was analyzed using FTIR.
International Journal of Environmental Science and Technology (2022) 19:4019–4036 4031

Table 5  Composition of the S/No. Retention time (min) Hydrocarbons Wt%

catalytic oil fraction distilled in
the gasoline range 1 2.09 Butyl cyclopropane 0.99
2 2.14 Heptane 4.97
3 2.35 2,4-Hexadien-1-ol 0.70
4 2.42 3,7-Dimethyl-1,6-octadiene 0.60
5 2.73 1,5-Heptadien-3-yne 1.89
6 2.94 1,6-Heptadien-3-yne 5.77
7 3.06 3-Ethyl-hexane 6.36
8 3.58 2,4-Dimethyl-1-heptene 2.98
9 4.45 2-Nonene 6.96
10 4.64 2-(3-butynyloxy) Tetrahydro pyran 6.96
11 5.92 Benzaldehyde 0.40
12 6.28 2-Nonyn-1-ol 1.99
13 6.50 7-Tetradecene 7.26
14 6.80 Decane 7.85
15 8.97 8-Tetradecene 8.15
16 9.24 1,2-Epoxynonane 8.35
17 11.44 3-Dodecene 3.98
18 11.65 1-Methylpentyl cyclopropane 4.17
19 13.79 6-Tridecene 2.78
20 14.00 2-Methyl undecane 2.98
21 16.07 3-Dodecene 2.39
22 16.25 Tetradecane 1.99
23 18.25 5-Dodecene 1.79
24 18.42 2,6,10,14-Tetramethyl heptadecane 0.40
25 20.33 2-Hexadecen-1-ol 1.29
26 20.49 2-Methyl heptadecane 1.19
27 22.32 4-Hexadecen-1-ol 0.80
28 22.46 3-Methyl tridecane 0.99
29 24.22 9-Hexadecen-1-ol 0.50
30 24.35 2,6-Dimethyl heptadecane 0.70
31 26.03 3-Tetradecene 0.20
32 26.15 2,6,10,14-Tetramethyl heptadecane 0.40
33 27.76 7-Tetradecene 0.20
34 27.87 2,6,10-trimethyl dodecane 0.30
35 29.28 2,6,10,15-Tetramethyl heptadecane 0.50
36 32.82 2,2-Dimethyleicosane 0.30

The IR spectra of Fe catalyzed and non-catalytic par-
ent oils are given in Fig.  10. The peaks at 2854  ­c m −1,
2925 ­cm−1 and 2959 ­cm−1 indicate C–H stretching, and
the peak at 1454 ­c m −1 shows C–H bending in alkanes.
The peak at 3082 ­cm−1 represents = C–H stretching, while
the peaks at 1697 ­c m −1 and 1643 ­c m −1 represent C=C
stretching in alkenes. Similarly, the bands at 910 ­c m −1
and 709 ­cm−1 show = C–H bending in alkenes. The peak
at 3082 ­cm−1 represents aromatic = C–H stretching. The
peaks at 1589 ­cm−1, 1454  ­cm−1 and 1417 ­cm−1 are due
to aromatic C–C stretching. The peaks at 910 ­cm−1 and
709  ­c m −1 are due to out-of-plane bending in aromatic
rings.
It is noteworthy that the spectrum of Fe catalyzed oil is
having a broad peak in the region 3500–3200 ­cm−1, indi-
cating a difference from that of the non-catalytic oil. This
broad peak shows O–H stretching of alcohols (Donal et al.
2009). The GC–MS study also shows that alcohols have
been produced abundantly in the Fe-catalyzed parent oil
as evident from Table 3. It can be observed that alcoholic

13

4032
Fig. 14  Chromatogram of catalytic oil fraction obtained in the kerosene range
hydrocarbons like 1,7-heptanediol (S.No. 4), 1-hexade-
canol (S. No. 29), 2-butyl-1-octanol (S. No. 31), 1-hep-
tacosanol (S. No. 40) and 2-methyl-1-butanol (S. No. 42)
are present in the catalytic oil with relative abundance of
0.30%, 1.81%, 3.11%, 1.41% and 0.30%, respectively, but
these compounds are not present in the non-catalytic oil.
GC–MS characterization
The GC–MS characterization indicates that paraffins, ole-
fins, alkadienes and their branched and cyclic hydrocarbons
with alcohols, ketones and carboxylic derivatives are pre-
sent in the Fe-catalyzed parent oil as shown in Table 3 and
Fig. 11. The chromatogram given in Fig. 12 indicates the
hydrocarbons present in the non-catalytic parent oil which
are enlisted in Table 4. The results show that the non-cat-
alytic oil is comprised of mostly branched chain alkanes
and alkenes, and the cyclic compounds and alcohols are
seemed to be very low in concentration as compared to the
Fe-catalyzed oil. The non-catalytic oil contains aldehydes,
and the catalyst has favored formation of ketones. The
overall examination shows that the Fe-catalyzed parent oil
contains relatively lighter hydrocarbons as compared to the
13
International Journal of Environmental Science and Technology (2022) 19:4019–4036
non-catalytic parent oil. Similar results have been recorded
in the literature where formation of lighter hydrocarbons
with cyclic and branched chain structure has been favored by
the catalytic process as compared to the non-catalytic pro-
cess (Gulab et al. 2015). The GC–MS analysis of the cata-
lytic oil fraction obtained in gasoline range (Fig. 13) shows
mainly a hydrocarbon distribution over a range of ­C7–C19
with normal, branched and cyclic alkanes and alkenes, and
their derivatives as given in Table 5.
The chromatogram of the catalytic oil fraction distilled
in kerosene range shows a shift in the peaks toward higher
hydrocarbons as compared to the gasoline range (Fig. 14).
The hydrocarbons are distributed over a range of ­C7–C35
with an increasing trend in abundance up to retention time
of 22.75 and then decreasing gradually. Relatively higher
hydrocarbons can be observed in this fraction as compared
to the gasoline range fraction. This fraction is composed
of hydrocarbons having single and double bonds as well as
alcoholic and aromatic compounds (Table 6).
The chromatogram shown in Fig. 15 indicates hydrocar-
bons present in the catalytic oil fraction obtained in the die-
sel range. This fraction contains hydrocarbons distribution in
the range of C­ 12–C54 with constituent compounds exhibiting
International Journal of Environmental Science and Technology (2022) 19:4019–4036 4033

Table 6  Composition of the S/No. Retention time (min) Hydrocarbons Wt%

catalytic oil fraction distilled in
the kerosene range 1 6.33 Heptyl hydroperoxide 0.08
2 6.52 2,4,6,8-Tetramethyl-1-undecene 0.04
3 8.71 Allyl methyl ether 0.24
4 9.92 1-Butyl-2-hexanone 0.16
5 11.25 1-Decene 0.96
6 11.48 2-Phenyl bicyclo hept-2-ene 1.20
7 13.77 7-Tetradecene 1.92
8 14.02 2-Methyl undecane 2.88
9 16.23 5-Tetradecanol acetate 3.84
10 16.42 Tetradecane 4.40
11 18.49 2-Methyl-7-hexadecene 4.88
12 18.67 2,6,10-trimethyl dodecane 5.36
13 20.61 2-Hexyl-1-decanol 5.52
14 20.77 2,6,10-Trimethyl tetradecane 5.92
15 22.59 4-Methyl-7-hexadecene 5.36
16 22.75 2-Methyl-1-hexadecanol 6.00
17 22.94 2-Hexadecacen-1-ol 1.12
18 24.46 1-Eicosene 4.16
19 24.61 Octadecane 5.76
20 24.81 7-Octadecene 1.44
21 26.24 5-Nonadecene 4.08
22 26.38 Eicosane 5.28
23 26.59 3-Eicosene 1.04
24 27.88 Heptacosane 3.28
25 28.06 Heptacosane 4.72
26 28.28 1-Eicosene 0.96
27 29.53 10-Heneicosene 2.88
28 29.67 Heneicosane 4.16
29 29.91 17-Pentatriacontene 0.56
30 31.09 1-Docosene 2.24
31 31.22 Heptacosane 3.68
32 32.59 1-Heneicosyl formate 1.52
33 32.71 Hexacosane 3.20
34 32.96 17-Pentatriacontene 1.12

double ring, substituted benzene, alcohols and carboxylic
acids in addition to alkanes and alkenes (Table 7).
Conclusion
It can be concluded from the present study that the PET can
be effectively converted into liquid product in combination
with the LDPE and HDPE under the influence of Fe catalyst
at 500 °C in a 60-min reaction, while separately it cannot be
converted into liquid. A 20 g initial mass of the reactant was
found to be more effective, and the optimum mixing ratio
of the LDPE, HDPE and PET was found as 40%, 40% and
20%, respectively. Under the optimum conditions, the Fe
catalyst produced relatively higher yield of oil and resulted
in higher total % conversion as compared to the non-cata-
lytic reaction. The ASTM distillation shows that catalytic oil
contains relatively lighter hydrocarbons as compared to the
non-catalytic oil. The FTIR spectra of the catalytic oil show
difference in 3500–3200 ­cm−1 region due to the presence of
alcohols. The physicochemical properties of the catalytic
parent oils are in good agreement with that of the standard

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4034 International Journal of Environmental Science and Technology (2022) 19:4019–4036

Fig. 15  Chromatogram of the catalytic oil fraction obtained in the Diesel range

Table 7  Composition of the S/No. Retention time (min) Hydrocarbons Wt%

catalytic oil fraction distilled in
the diesel range 1 9.21 3-Dodecene 0.79
2 9.23 3-Methyl tridecane 1.18
3 10.75 7-Tetradecene 1.77
4 10.87 6-Tridecene 1.38
5 12.26 9-Hexadecen-1-ol 3.15
6 12.37 2-Hexyl-1-decanol 3.54
7 13.70 10-Methyl-8-tetradecen-1-ol acetate 5.91
8 15.10 2,3,5,6-tetramethyl bibenzyl 6.89
9 16.54 9-Hexadecenoic acid 2.17
10 17.59 Hexaethylidene cyclohexane 1.97
11 18.58 5,8,11,14-Eicosatetraynoic acid 2.76
12 19.61 5,5-Diallyl-2,2-biphenyldiol methyl ether 4.13
13 21.69 Cyclopenta anthracene-8,11-dione 1.57
14 22.84 Lycoxanthin 5.71
15 24.24 3,15-Octadecadien-1-ol acetate 5.91
16 25.79 Nonacosane 4.92
17 27.70 17-Pentatriacontene 5.71
18 28.89 Triacontane 5.91
19 30.40 Tetratriacontane 5.12
20 32.12 Heptacosane 4.92
21 34.14 Hexatriacontane 4.53
22 35.84 Tetracontane 4.53
23 37.37 Tetratetracontane 4.33
24 39.09 Nonacosane 3.35
25 41.01 Tetratetracontane 2.76
26 43.27 3-Ethyl-5-(2-ethylbutyl) octadecane 1.97
27 45.96 9-Cyclohexyl eicosane 1.57
28 49.17 Octadecanal 0.98
29 53.05 Tetrapentacontane 0.59

13
International Journal of Environmental Science and Technology (2022) 19:4019–4036 4035
fuels. The distilled fractions of the catalytic parent oil are in
close resemblance in their physicochemical characteristics to
the standard gasoline, kerosene and diesel oil. The GC–MS
analysis showed that the parent oil fraction distilled in gaso-
line range contains hydrocarbons in the range C ­ 7–C19, while
the kerosene range fraction is possessing hydrocarbons rang-
ing from C­ 7–C35 and the fraction distilled in diesel range is
having ­C12–C54 hydrocarbons. The PET individually under
the above conditions could not be converted to oil either in
catalytic or non-catalytic reactions.
Acknowledgments  Facilities provided by the Advanced Research
Laboratory of the Bacha Khan University Charsadda are highly
acknowledged.
Author contributions  All the authors contributed to the study con-
ception and design. Material preparation, data collection and analysis
were performed by SM, HG, KH, MH and MAH. The first draft of the
manuscript was written by SM, refined by the other authors and final-
ized by the corresponding author.
Funding  The authors did not receive any specific grant from any organ-
ization for accomplishing the present work.
Declarations  inesc​encia/​Infra​red%​20Spe​ctros​cop1.​pdf. Accessed 15 June 2018
Conflict of interest  The authors have no conflict of interest to be de-
clared related to the contents of this article.
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