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Optimization of The Pyrolysis Process of A Plastic Waste To Obtain A Liquid
Optimization of The Pyrolysis Process of A Plastic Waste To Obtain A Liquid
Optimization of The Pyrolysis Process of A Plastic Waste To Obtain A Liquid
A R T I C LE I N FO A B S T R A C T
Keywords: This study examines the possibility of using plastic film waste presented in municipal solid waste as a fuel. There
Polyethylene film is a large amount of this waste that is currently not treated and ends up in landfills aggravating the global
Plastics pyrolysis problem of marine and land pollution. A pyrolysis process was performed on this plastic waste to obtain a liquid
Polynomial modelling fuel. For this, an experimental design was carried out, varying the operating conditions. The physical and
Neural fuzzy modelling
chemical characteristics of the fuel, such as liquid fraction yield and higher calorific value, were determined and
a statistical analysis has been carried out using polynomial and neural fuzzy models. In all the adjustments an r2
greater than 0.95 was obtained and the neural fuzzy model fit the experimental data better than the polynomial
model. The optimum operating conditions for the production of this oil are: a temperature of 500 °C, a residence
time of 120 min, and 20 °C/min of heating rate.
1. Introduction were recovered for recycling, resulting in a poor recycling ratio. Fur-
thermore, less than 17% was recovered energetically and more than
Polymers are an integral part of the global economy. While they 46% of the plastic waste was landfilled [1].
bring numerous benefits to society, they also come with disadvantages, Plastic materials are a very efficient resource in many sectors
since many plastic materials are used only once and discarded, thus (packaging, construction, automotive, electric, agriculture, etc.) and
losing 95% of their value. Poor management of plastic materials causes they can help to reduce CO2 emissions and save energy. Energy con-
many problems. One of them is the large amount of oil needed, between sumption and greenhouse gas emissions would increase significantly if
4% and 6% of global production every year [1,2]. Other problems in- plastic products were replaced by other materials. In other words,
clude greenhouse gases emissions and the dumping of waste into seas substituting more traditional materials with a plastic product can help
[3]. Greenhouse gas emissions are generated primarily as a result of reduce energy consumption and the emission of greenhouse gas [4].
energy consumption in the plastics processing industry [4]. However, for the full potential of these plastic products to be rea-
Possibly the biggest problem is the amount of plastic waste gener- lised, at the end of their useful life they must be turned into a new
ated. The total plastic production in the world was around 335 million resource. Thus it becomes vitally important to promote mechanical and
tons in 2016, of which 60 million tonnes were produced in Europe [5]. chemical recycling and to avoid depositing the plastic waste into
After the useful life of plastic products, many are collected as plastic landfills [6]. The oil obtained through the pyrolysis of plastic waste is a
waste which can either be further treated, recycled, or discarded, often valuable source of fuel [7].
into landfills or the ocean. In Europe in 2016, 27.1 million tonnes of In this paper non-catalytic pyrolysis has been proposed as an al-
post-consumer plastic waste were collected for further treatment, more ternative processing of a plastic waste in order to avoid placing the
than 27.3% of plastic waste was deposited in landfills, 31.1% of plastics waste in a landfill. Many authors such as Sharuddin et al. [8], Al-Salem
waste was recycled and 41.6% was recovered energetically. Although et al. [9], Dermibas [10], Kumari and Kumar [11], Sogancioglu et al.
the situation in the EU is improving, landfilling is still, in many coun- [12] and Syamsiro et al. [13], have studied the pyrolysis of plastic
tries, the first option for post-consumer plastic waste treatment, as is the waste, but few authors have studied plastic film from municipal solid
case in Spain. In Spain, 2.3 million tonnes of post-consumer plastics waste, which had not been collected selectively. This fraction of mu-
waste were collected for further treatment. Only 0.8 million tonnes nicipal solid waste is a mixture of different plastic products [14],
⁎
Corresponding author.
E-mail addresses: lucia9s@ugr.es (L. Quesada), aperezm@ugr.es (A. Pérez), vgcalero@ugr.es (V. Godoy), fpeula@rethinking.ong (F.J. Peula),
mcaleroh@ugr.es (M. Calero), gblazque@ugr.es (G. Blázquez).
https://doi.org/10.1016/j.enconman.2019.03.054
Received 14 January 2019; Received in revised form 6 March 2019; Accepted 19 March 2019
Available online 25 March 2019
0196-8904/ © 2019 Elsevier Ltd. All rights reserved.
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
2.1. Materials
Liquid and solid fractions were collected.
The experiments carried out and their corresponding operating
The plastic material studied in this work was collected from a me-
conditions are shown in Table 2.
chanical-biological treatment plant of municipal solid waste located in
Alhendín (Granada), Spain. This plastic waste was not collected selec-
2.3. Determination of liquid fraction yields (ƞoil)
tively. The plastic waste was 100% film and mainly formed by poly-
ethylene (PE). First a characterization was made at the treatment plant
After the pyrolysis process, the yield of the liquid fraction was de-
(Alhendín), where several samples were taken from the bunker of the
termined by weight difference using the following equation,
film. After this, a series of separations were made in order to isolate the
PE to perform the experiments in the laboratory. The composition of the OWf
ηoil = ∗ 100
waste was found to be 86% polyethylene, 6.7% PP, 3% paper-cardboard OWi (1)
and 4.3% plastic containers and impurities (mainly organic matter).
where:
Pellets were used to carry out the pyrolysis experiments because the
film was incompatible with the reactor dimensions. To manufacture the
owf, final weight of oil
pellets, the film was washed, dried and pelletized. The final size of the
owi, initial weight of polymer
pellets was 3–4 mm and the moisture content was less than 1%, ac-
cording to UNE-EN 18134–3:2016.
2.4. Determination of char yields (ƞchar)
2.2. Pyrolysis test After the pyrolysis process, the yield of the char was determined by
weight difference using the following equation,
For pyrolysis tests, a horizontal tubular reactor of Naberthem was
used [22]. Dimensions of this reactor are shown in Table 1 Approxi- CWf
ηchar = ∗ 100
mately 40 g of sample were used for each experiment and a constant CWi (2)
nitrogen flow rate of 50 l/h was used to ensure an inert atmosphere. where:
A total of 15 experiments were carried out in the reactor. The ob-
jective of these experiments was to determine the effect of three op- cwf, final weight of char
erational variables: temperature, residence time and heating rate. cwi, initial weight of polymer
Table 1
2.5. Higher calorific value of liquid fraction
Reactor dimensions.
Finally, using the data obtained from the oil yield and higher ca-
External dimensions, mm Tube outside diameter, mm Tube length, mm lorific value, the energy yield was calculated using the following
equation,
Width Depth Height
ηenergy = HCV ∗ ηoil (3)
434 340 508 50 450
In this paper the energy yield is understood as the amount of energy
20
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
that is obtained from the oil in relation to the amount of material that is time), a5
used. R6 → (intermediate temperature, low heating rate, high residence
time), a6
2.7. Experimental design R7 → (intermediate temperature, high heating rate, low residence
time), a7
Through factorial design, an empirical model with a series of in- R8 → (intermediate temperature, high heating rate, high residence
dependent variables (temperature, residence time, heating rate) was time), a8
studied to establish liquid oil yield, char yield, higher calorific value R9 → (high temperature, low heating rate, low residence time), a9
and energy efficiency. For this purpose, a central composition factorial R10 → (high temperature, low heating rate, high residence time), a10
design was used. The values were normalized between −1 and 1. R11 → (high temperature, high heating rate, low residence time), a11
The design used is defined by three parameters: number of vari- R12 → (high temperature, high heating rate, high residence time),
ables, k; constant, p, which takes the values 0 for k < 5 and 1 for a12
k > 5; and number of central points, nc. Examinations of the central
points will be performed in triplicate in order to obtain average values. μlFi (xi, Θi1) Gaussian dependency function, which is the combina-
These parameters represent three groups of points: tion of the three levels (low, medium and high) for each independent
variable, where xi are independent variables (temperature, heating
- 2 k-p points constituting a factorial design. rate, residence time).
- 2*k axial points. Determination of Gaussian dependency function was possible using
- nc central points. the following equation [20].
21
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
Table 3
Experimental results for liquid fraction yield, neural fuzzy model data and polynomial model data.
Test Ƞoil exp, % Ƞoil neural fuzzy, % Ƞoil polyn, % Coefficients, neural fuzzy Coefficients, polynomial
22
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
Table 4
Experimental results for char yield, neural fuzzy model data and polynomial model data.
Test Ƞchar exp, % Ƞchar neural fuzzy, % Ƞchar polyn., % Coefficient, neural fuzzy Coefficient, polynomial
average values of 7% of char for PE and Sarker et al. [32] who obtained
average values of 5% of char for mixed plastics. Similarly, other authors
such as Symasiro et al. [13] obtained 14% of char for municipal plastic
waste.
It should be noted that, in the experiments carried out at 450 °C and
40 min, the pellets have not been completely degraded due to the low
temperature and the short residence time. For this reason, the value of
char yield obtained has not been taken into account.
The highest char values were obtained experimentally at inter-
mediate residence times, so the residence time variable is the one that
most greatly influences this parameter. However, the temperature
variable and the heating rate also affect this parameter considerably in
combination with the residence time. In order to study the influence of
the process variables on the yield of char obtained, the adjustments
were made using the ANFIS and the polynomial model.
Table 4 shows all the parameters obtained in the adjustment to the
ANFIS model and Fig. 2.a shows the char yield obtained in relation to
temperature and residence time, keeping the heating rate constant. An
r2 value of approximately 1 was obtained which verifies that this model
is a good fit for the data in the range of study. In this case, the negative
variables obtained lose their physical meaning.
Residence times of 80 min and 120 min resulted in the highest for-
mations of char, however the purpose of the study is to high liquid
fraction. Constants a1 and a4 were identified as the optimal values.
When working at low temperature, low heating rate and low residence
time (a1) 0% char was obtained and when working at low temperature,
high heating rate and high residence time (a4) 0% char was also ob-
tained. Temperature and residence time are the most important factors
while heating rate has little importance. At low temperature, residence
time has a greater influence.
Table 4 shows all the parameters obtained in the adjustment to the
polynomial model and Fig. 2.b shows the char yield in relation to
temperature and residence time. It can be seen that the surface has the
same trend as in the previous case but it is more rigid and its profile less
adapted to the real results.
It is seen that the coefficient of the residence time and temperature
are of greater importance and, therefore, these are the variables that
most influence yield. The coefficient of the quadratic term of residence
time is negative (−2.90828); the value is highest in the middle level Fig. 2. Char yield as a function of temperature and time: a) neural fuzzy model;
(when the normalized variable is 0). In relation to the synergy of time b) polynomial model.
with the other variables, it is negative and of little importance in terms
of heating rate (−0.669375), whereas the synergy of time with tem- 3.3. Higher calorific value (HHV)
perature is very important with a term of −2.06237. Lastly the coef-
ficient of the temperature term is positive (1.3886) and has great in- Table 5 shows the higher calorific value (HHV) of liquid fraction for
fluence on the extreme conditions. each experiment. The average HHV was 10.9 kcal/g. These results were
higher than those obtained by other authors, for example Syamsiro
et al., [13] studied the calorific value of polyethylene bags, obtaining a
23
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
Table 5
Experimental results for higher calorific value, neural fuzzy model data. And polynomial model data.
Test HHV exp, kcal/g HHV neural fuzzy, kcal/g HHV polyn, kcal/g Coefficients, neural fuzzy Coefficients, polyn.
value of 9.9 kcal/g. Ahmad et al. [33] obtained a value of 9.67 kcal/g
for HDPE, Desai and Galage [34] determined the HHV for LDPE, to be
9.43 kcal/g and Sharuddin et al. [35] obtained a liquid with an HHV of
around 9.6 kcal/g. In addition, the average higher calorific values ob-
tained in the series of experiments carried out in this research were
higher than those for diesel, 10.7 kcal/g and biodiesel, 8.8 kcal/g [36].
This may be due to the fact that the liquid fraction recovered, was not
cracked, and therefore light and heavy naphtha were found in the
characterized fraction.
There is no clear difference between the HHVs obtained, but a slight
tendency for the highest calorific value to be at intermediate tem-
perature (500 °C), is observed. The variable that most affected the ca-
lorific value was temperature, while residence time and the heating rate
have less influence. In order to determine the influence of the process
variables on the HHV, adjustments were made using both models.
Table 5 shows all the parameters obtained in the adjustment to a
neural fuzzy model and Fig. 3.a shows the higher calorific value ob-
tained in relation to temperature and residence time, keeping the
heating rate constant. A good fit of the model was verified with an r2 of
0.98. The optimal value of the constant a6 is 11.42 kcal/g which verifies
that the optimum operating conditions were at intermediate tempera-
ture and at high residence time.
Table 5 show all the parameters obtained in the adjustment to the
polynomial model and Fig. 3.b shows the higher calorific value in re-
lation to temperature and residence time. In this case, the surface is
more rigid and less adapted to the experimental values but maintains
the shape of the previous case.
The polynomial model shows that the coefficients of the tempera-
ture and heating rate are of greater value than those of residence time.
With respect of to the quadratic terms, the temperature (−0.0644062)
and the heating rate (−0.0327563) have a negative value thus the
optimum value of these parameters is in the middle level. In regard to
residence time, the quadratic value is positive so the optimum value of
this is in the extreme values, yet note that residence time had only
minor effects on product composition. With respect to the synergies, the
most important is the temperature and the heating rate, being this
positive and optimal to high values of the variables. Fig. 3. Higher calorific value as a function of temperature and time: a) neural
fuzzy model; b) polynomial model.
24
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
Table 6
Experimental results for energy efficiency, neural fuzzy model data and polynomial model data.
Test Ƞenergy exp., kcal/g Ƞenergy neural fuzzy, kcal/g Ƞenergy polyn, kcal/g Coefficient, neural fuzzy Coefficient, polynomial
4. Conclusions
25
L. Quesada, et al. Energy Conversion and Management 188 (2019) 19–26
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