Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

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Biocatalysis and Agricultural Biotechnology

journal homepage: www.elsevier.com/locate/bab

Effect of processing parameters on cellulose content extracted

from pineapple leaf
M.S. Abdul Karim a, N. Zainol a, *, N.I.A. Abu Hassan As’ari a, N. Abu Talip Yusof a, b,
N.H. Aziz a
a
College of Engineering, Universiti Malaysia Pahang, Lebuhraya Tun Razak, 26300, Gambang, Kuantan, Pahang, Malaysia
b
Centre for Research in Advanced Fluid & Processes (Fluid Centre), Universiti Malaysia Pahang, Lebuhraya Tun Razak, 26300, Gambang, Kuantan,
Pahang, Malaysia

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

Keywords: The development of dielectric materials from natural fibers of high cellulosic materials could
Pineapple leaf potentially reduce environmental pollution and human health risk due to their biodegradability
Soda pulping and non-carcinogenic properties. Comprehending the important process parameters is always
Cellulose content challenging in material development to produce a dielectric material with great performance.
Factorial analysis Therefore, this research aims to evaluate the effect of processing parameters on cellulose
Permittivity
extraction from pineapple leaves and determine the most significant parameters contributing to
the extraction process and its corresponding permittivity value. The soda pulping method was
used in cellulose extraction, and the content was analyzed by the Kurschner-Hanack method. The
one-factor-at-a-time analysis was adopted to study the effect of pulping time on cellulose content
while keeping the other parameters constant. The two-level factorial analysis was used to
determine the significant parameters and the best conditions for the cellulose extraction with
pineapple leaf to soda ratio (1:5 and 1:10), soda concentration (5 and 10 wt%), temperature (60
and 100 ◦ C), and pulping time (46–75 min) as processing parameters. The results showed that the
pineapple leaf to soda ratio was the most significant parameter in cellulose extraction. A
maximum cellulose value of 40.51% was obtained at 1:5 pineapple leaf to soda ratio, 10 wt% soda
concentration, 100 ◦ C temperature, and 75 min of pulping time, contributing to a 1.6626
permittivity value. Therefore, the best extraction conditions and significant process parameters
determined in this study can be used to tailor the parameters to the desired conditions for a higher
cellulose yield and permittivity value.

1. Introduction
The booming demand for fresh fruits with increasing population density has caused an upsurge in recent consumption patterns.
Rich in vitamins and fibers, pineapple (Ananas comosus) is among the fresh fruits in continuous supply and demand across the globe.
Pineapple presents the most promising fruit demand in Malaysia’s domestic and export markets (Nazri and Pebrian, 2017), as proven
by its substantial plantation areas of more than 17,601 ha (Jenny, 2018). It is also ranked second after mango as the most important
tropical fruit, followed by papaya and avocado (Altendorf, 2019). Pineapple is the most traded tropical fruit globally. Its consumption
is projected to grow in the coming years due to rising household incomes and population growth coupled with the rapid expansion of

* Corresponding author. /
E-mail address: azwina@ump.edu.my (N. Zainol).

https://doi.org/10.1016/j.bcab.2022.102339
Received 18 January 2022; Received in revised form 11 March 2022; Accepted 30 March 2022
Available online 1 April 2022
1878-8181/© 2022 Elsevier Ltd. All rights reserved.
M.S. Abdul Karim et al. Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

global markets.
Pineapples can be eaten as fresh fruit or processed to produce canned pineapple, juice, and food spreads. These processed food
products and post-pineapple harvesting lead to biomass waste such as pineapple leaves, crowns, and cores. The generation of pineapple
waste may contribute to environmental pollution as it is commonly burnt in the open air or left to rot on the ground (Zainuddin et al.,
2014). This happens due to the expensive disposal method, which comes from the high transportation costs and limited landfill
availability (Upadhyay et al., 2013). Inefficient disposal methods could further negatively affect human health since they require
time-consuming degradation of the wastes, which consequently attracts pests during the degradation process. Furthermore, the high
biological oxygen demand (BOD) and chemical oxygen demand (COD) (Ban-Koffi and Han, 1990) in the pineapple wastes further
added to the difficulties of the disposal process. Another method of disposing of pineapple waste is through vermicomposting, which
results in the rapid decomposition of pineapple pulp and peel. However, the cost-effectiveness has yet to be confirmed (Mainoo et al.,
2009). Exploiting pineapple waste into a value-added product seems to be the most practical way to manage its waste, thereby leading
to environmental friendliness. Hence, with sustainable utilization of these wastes, valuable products could be derived from pineapple
wastes.
The pineapple wastes, particularly the leaf parts, consist of highly cellulosic fibrous materials that function for extra-specific
strength and stiffness (Asim et al., 2015). These include cellulose, hemicellulose, holocellulose, and lignin (Daud et al., 2015). The
cellulose content in pineapple leaf fiber is the highest at 81.27%, followed by hemicellulose at 12.31% and 3.46% lignin (Cherian et al.,
2010). The low lignin composition in the pineapple leaf fibers is advantageous for chemical extraction since lignin functions as an
adhesive that binds cellulose and hemicellulose (Daud et al., 2015). Cellulose is primarily used in paper-making and textile
manufacturing (Asim et al., 2015; Dinh Vu et al., 2017; Mahardika et al., 2018). Its strength and stiffness properties also make it useful
as a reinforcing material (Dinh Vu et al., 2017; Mahardika et al., 2018). Additionally, cellulose has also been used as raw material to
produce biofuel (Chen et al., 2019; Rajnish et al., 2021). Currently, the use of natural fibers in dielectric material development seems to
be getting the spotlight in the materials engineering industry. Due to their non-carcinogenic and biodegradability features, natural
fibers can be exploited as an alternative to conventional dielectric materials such as alumina, mica, and Teflon, which are widely used
in electrical and electronic applications such as capacitors, insulators, printed circuit boards, and antennas.
Recognizing the potential of cellulose from natural fiber-based as an alternative method for producing new-developed dielectric
materials, several different methods are reported for cellulose extraction. These include hydrothermal, wet oxidation, organosolv,
acidic, soda (alkaline), sulfate, ammonia fiber explosion, ionic liquid pretreatment method, and soda-oxygen pulping (Dinh Vu et al.,
2017; Yue et al., 2016). Soda pulping, also known as an alkaline treatment, is a simple extraction method that requires suitable pa­
rameters during the extraction process for maximum cellulose yield. The cell wall of the fibers is disrupted during the treatment
process through the hydrolyzation of acetic acid and uronic acid esters, resulting in swollen cellulose and dissolved lignin, hemicel­
lulose, and silica (Dinh Vu et al., 2017). The soda pulping method is less reactive towards cellulose than other methods such as sulfate
pulping. Sulfate pulping causes the cellulose to be more reactive (Bajpai, 2018), which is undesirable. Unlike soda pulping, the other
extraction methods are energy-intensive and rather expensive, apart from chemical utilization, which requires special handling,
disposal, or production methods. Another upgraded method of soda pulping, known as soda-oxygen pulping, requires oxygen, which
further assists the extraction process. Even though requiring less energy due to the low pulping temperature requirement, this method
is complicated and involves heterogeneous reactions with various gas-liquid-solid states (Yue et al., 2016).
Several parameters are known to affect cellulose yields during the extraction process from different types of plant wastes. Melikoğlu
et al. (2019) studied the effects of sodium hydroxide (NaOH) concentration, temperature, and extraction time on cellulose nanocrystal
extraction from apple waste through an alkaline treatment method. Dinh Vu et al. (2017) investigated the effect of temperature and
alkaline concentration assisted with ultrasound irradiation to reduce the extraction time of cellulose from rice straw. Liu and Wang
(2016) applied an acid treatment method for the extraction of cellulose from wheat bran. The parameters involved include hydrogen
peroxide concentration, liquid-solid ratio, temperature, reaction time, and ultrasonic pretreatment power. While in the study of
cellulose extraction from sugarcane bagasse by Bektashi et al. (2020), the selection of parameters included delignification pH, sodium
chlorite (NaClO2) concentration, and solvent ratio. Nevertheless, the three most important parameters reported to be effective on the
cellulose yield during the extraction process in the alkaline treatment method are alkaline concentration, pulping time, and tem­
perature (Rodsamran and Sothornvit, 2015).
An analysis of the effect of parameters on cellulose yields can be done by using a one-factor-at-a-time (OFAT) analysis. OFAT
analysis can be used to determine the effect of one parameter in the cellulose extraction process by varying only one parameter while
keeping the other parameters constant (Abou-Taleb and Galal, 2018). The determination of the effect of one parameter on the process
is very necessary to fully understand the process for maximum yields. Other than that, factorial analysis (FA) has also become one of
the best alternatives to determine the number of parameters influencing variables and analyze which variables are best suited to each
other. FA is a way to condense data in many variables into fewer variables rather than focusing on many variables that may be
insignificant. Hence, the use of FA is important in analyzing the influence of several parameters that contributed to cellulose extraction
from the pineapple fibers from their leaf by evaluating all the parameters involved. Inadequate knowledge of the most important
parameters influencing cellulose extraction will be a major concern for that extraction process.
Acknowledgment of the most influential parameters for tailoring the parameters involved during the extraction process in order to
maximize cellulose yield is very important. It is crucial to fully understand the parameters that significantly affect the process. The two-
level factorial analysis (TLFA) can be applied to evaluate the most significant parameters and identify the interactive parameters
simultaneously. Although there is plenty of research work on cellulosic materials, only a few studies are available on the permittivity
(ϵ) of raw cellulose. Most of the research on pineapple leaf fibers focused on the application of cellulose in paper production and as a
reinforcing material in composites. Therefore, this study was conducted to determine the effect of processing parameters on cellulose

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M.S. Abdul Karim et al. Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

extraction through the soda pulping method and its corresponding permittivity value. This study also aimed to determine the most
significant parameters affecting cellulose extraction and the best extraction conditions for maximum cellulose yields. In this study,
cellulose extraction was conducted using a soda pulping method. Four parameters were chosen in this study, including pineapple leaf
to soda ratio (PL:S), soda concentration, temperature, and pulping time. The outcome of this study is expected to be able to identify the
most influential parameters on the cellulose content value. Suitable modifications of these processing parameters during the extraction
process could remarkably enhance yields, thereby increasing their permittivity value.

2. Materials and method

2.1. Collection of samples
Pineapple leaves (PL) were used in this study as a raw material. The PL was collected from a pineapple plantation located at Pekan
Pina, Pekan, Pahang, Malaysia.

2.2. Soda pulping experiment and cellulose content analysis

Fig. 1 illustrates the sample preparation procedure for cellulose extraction and permittivity tests. This work adopted the soda
pulping method for cellulose extraction from PL. The harvested leaves were initially cleaned with tap water to remove dirt. The leaves
were dried in an oven at 100 ◦ C for 20 min before being cut into smaller pieces of approximately 2 cm long. In this research, sodium
hydroxide was used as the soda for pulping. The soda was mixed with PL in a beaker until submerged. The beaker was then placed on
the hot plate before being heated. A glass rod was used to manually stir the mixture five times every 15 min. The cool-cooked mixture
was filtered and blended until it became pulp. The pulp was thoroughly washed with water until a clear residue was obtained before
being squeezed. The squeezed pulp was then dried in an oven at 60 ◦ C to obtain the dried pulp. Cellulose content analysis and
permittivity tests were conducted on the dried pulp.
The cellulose content in the pulp was determined by Kurschner’s and Hanack’s methods (Moshi et al., 2019). This method uses
acetic acid and nitric acid as the reagents. 1.5 ml of concentrated nitric acid and 15 ml of 80% acetic acid were prepared. Both reagents
were added into a beaker containing 1 g of air-dried pulp, and the mixture was heated to 100 ◦ C for 20 min. Next, the mixture was
filtered and washed thoroughly before being dried in an oven at 105 ◦ C for 24 h. The weight of the pulp was recorded to determine the
cellulose content (%) presence in the pulp, as mentioned by Meinert and Delmer (1977).

2.3. Dielectric material characterization

The developed samples were characterized using a G-band waveguide, which covers frequencies from 4 to 6 GHz with the fixed
height of TE10 mode. Thus, the sample must be prepared with the same height of 22.15 mm, but the width and length can be any
dimension as long as they can be fitted into the 47.55 mm G-band waveguide. With less restriction on the size of the sample, the sample
preparation process was easier. The experimental arrangement for the permittivity measurement is shown in Fig. 2. The complex
transmission parameter of S21 was measured by the Vector Network (VNA), where the waveguide was connected to the VNA by low-
noise coaxial cable and coax-to-waveguide adapters. As shown in Fig. 2, the sample as material under test (MUT) with a preferable
rectangular shape was partially placed at the center of the waveguide. The measurement of S21 can be done without prior calibration of

Fig. 1. Experimental procedure for soda pulping.

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M.S. Abdul Karim et al. Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

Fig. 2. Measurement setup for permittivity test of cellulose fibers.

the VNA since this technique utilizes the difference between empty and filled-with-sample measurement. The inverse technique was
utilized to estimate the permittivity of the S21 (Hasan et al., 2021; Karim et al., 2014).

2.4. Experimental setup for one-factor-at-a-time (OFAT) experiment

Pulping time was selected for the OFAT experiment since the range for the pulping time in TLFA will be decided based on OFAT’s
result. The selected range for the pulping time was between 15 and 75 min. While doing this experiment, the other parameters such as
pineapple leaf to soda ratio (PL:S), soda concentration, and temperature were fixed at 1:5, 10 wt%, and 60 ◦ C, respectively. For 1:5
pineapple leaves to soda, 100 g of pineapple leaves and 500 ml of soda were used. The soda concentration of 10 wt% was prepared by
dissolving 50 g of sodium hydroxide (NaOH) with 500 ml of distilled water. The temperature of 60 ◦ C was achieved using the hotplate
and was maintained by manually checking with a thermometer. Table 1 shows the OFAT experimental design generated by the Design-
Expert software. The cellulose extraction process was conducted based on Table 1 and the method mentioned in Part 2.2.

2.5. Experimental setup for two-level factorial analysis (TLFA)

Four parameters were chosen, including pineapple leaves to soda ratio (PL:S), soda concentration, temperature, and pulping time.
The 1:5 PL:S was prepared with 100 g of pineapple leaves and 500 ml of soda. Meanwhile, for 1:10 PL:S, 100 g of pineapple leaves were
mixed with 1000 ml of soda. In this work, 5% and 10% soda concentrations were prepared. To prepare the concentration, the mass of
NaOH was derived from the soda concentration using the following Equation (1):
Mass of sodium hydroxide (g)
Soda concentration (%) = × 100 (1)
Volume of solution (ml)
The cooking temperature was selected between the range of 60–100 ◦ C, and the temperature was adjusted using a hot plate and
manually checked with a thermometer. The mixture was stirred manually five times every 15 min. The pulping time was set at 45–75
min. This range was selected since results from the OFAT experiment showed that pulping times of less than 45 min were insignificant
for the cellulose extraction process.
The design of the experiment was performed with the aid of Design-Expert software, where all parameters were randomized, with
16 total runs. Each of the 16 runs has either the upper or lower limit of the four parameters. The results were analyzed by the Design-
Expert software to determine the most significant parameter and the interaction between the parameters. Table 2 shows the factorial

Table 1
OFAT experiment for pulping time effect on the cellulose extraction process.

Std Run Pulping time (min)

1 15
2 15
3 30
4 60
5 75
6 75
7 45

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M.S. Abdul Karim et al. Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

design table for the factorial analysis experiment. The cellulose extraction process was conducted based on Table 2 and the method
mentioned in Part 2.2.

2.6. Best condition validation experiment

The validation experiment was conducted according to the suggested best conditions obtained from data analysis of Design-Expert
software. The experiment was conducted to compare the suggested predicted data with the experimental data to determine the error
between experimental and predicted values. The formula for error calculation is as shown in Equation (2).
Predicted value − Experimental value
Error (%) = × 100 (2)
Predicted value
The permittivity was tested at the maximum and minimum cellulose content values based on Table 2. The morphology of the
maximum and minimum cellulose fibers of the developed samples was analyzed from the top view of scanning electron microscopy
(SEM; HITACHI/TM3030 PLUS, JAPAN) images.

3. Results and discussions

3.1. OFAT analysis on the cellulose extraction process
The effect of pulping time on cellulose content (%) was graphically portrayed in Fig. 3. The cellulose content was seen to gradually
increase from 15 to 75 min of pulping time. The figure depicted that the cellulose content could be improved with increasing pulping
time. The increase in pulping time resulted in more lignin being removed, so more cellulose could be obtained. The cellulose content
was the lowest at 15 min of pulping time since the cooking time was the shortest, indicating that the delignification process was just
about to occur. Meanwhile, at 75 min, the cellulose content was the highest due to the longer cooking time; hence, the delignification
process could occur longer (Cheng et al., 2011).
Table 3 summarizes the analysis of variance (ANOVA) for cellulose content. The function of ANOVA is to evaluate the coefficient of
the model, verify the significance of parameters, and determine the appropriateness of the chosen range. The confidence level por­
trayed by the ANOVA table was greater than 95%, while the p-value of the model was 0.0158. The p-value of the model was less than
0.05 and signified the significance of the model, implying its suitability for this experiment.
Equation (3) presents a second-order quadratic model established from the experimental data.

Cellulose content = 21.54638 + 0.069114A + 1.37E − 03A2 (3)

The equation correlates the interaction between input and output variables, with A representing the pulping time. The equation
was also used to understand the interactions between parameters (Zainol and Rahim, 2017; Zainol et al., 2017), which are the pulping
time and cellulose content. The R2 for this model was 0.8744, suggesting a good fit to the experimental data and could represent the
process. According to Ölmez (2009), R2 for a biological process should be at least 0.8.

3.2. TLFA of the cellulose extraction process

Table 4 presents 16 experimental runs with different processing conditions and the cellulose content (%). An ANOVA was used to
analyze the responses based on a 95% confidence level. The cellulose content in the samples ranges from 14.83% to 39.38%. The
lowest cellulose content was recorded in the pulping conditions of 1:10 PL:S, 5 wt% soda concentration, 100 ◦ C temperature, and 75
min of pulping time (Run 14). Meanwhile, the highest recorded cellulose content was obtained in an experimental condition of 1:5 PL:
S, 10 wt% soda concentration, at a temperature of 100 ◦ C and 75 min of pulping time (Run 15).

Table 2
Two-level factorial analysis experiment of the cellulose extraction process.

Std A: PL:S (g/ml) B: Soda concentration (wt.%) C: Temperature (◦ C) D: Pulping time (min)

1 1:5 5.00 60 45.00

2 1:10 5.00 60 45.00
3 1:5 10.00 60 45.00
4 1:10 10.00 60 45.00
5 1:5 5.00 100 45.00
6 1:10 5.00 100 45.00
7 1:5 10.00 100 45.00
8 1:10 10.00 100 45.00
9 1:5 5.00 60 75.00
10 1:10 5.00 60 75.00
11 1:5 10.00 60 75.00
12 1:10 10.00 60 75.00
13 1:5 5.00 100 75.00
14 1:10 5.00 100 75.00
15 1:5 10.00 100 75.00
16 1:10 10.00 100 75.00

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Fig. 3. Effect of pulping time (min) on cellulose content (%) from OFAT analysis.

Table 3
Analysis of variance for OFAT experiment.

Source Sum of squares Mean square F value p-value (Prob > F)

Model 152.1 76.05 13.92 0.0158

A- Pulping time 150.22 150.22 27.5 0.0063
A2 1.88 1.88 0.34 0.5891
Residual 21.85 5.46
Lack of fit 21.83 10.92 1091.67 0.0009

Table 4
Experimental results for two-level factorial analysis.

Run A: PL:S (g/ml) B: Soda concentration (wt.%) C: Temperature, (◦ C) D: Pulping time (min) Cellulose content (%)

1 1:5 5 60 45 23.81
2 1:10 5 60 45 20.98
3 1:5 10 60 45 25.62
4 1:10 10 60 45 24.93
5 1:5 5 100 45 23.86
6 1:10 5 100 45 27.81
7 1:5 10 100 45 22.36
8 1:10 10 100 45 22.44
9 1:5 5 60 75 32.1
10 1:10 5 60 75 22.2
11 1:5 10 60 75 19.16
12 1:10 10 60 75 20.59
13 1:5 5 100 75 19.15
14 1:10 5 100 75 14.83
15 1:5 10 100 75 39.38
16 1:10 10 100 75 23.11

3.3. ANOVA and significant parameters in the cellulose extraction process

Based on the analysis, the contribution percentage for each parameter was obtained, with PL:S presenting the highest percentage of
10.59% towards cellulose content. These were followed by soda concentration and temperature, with 2.15% and 0.15%, respectively.
Pulping time exhibited the least contribution to cellulose content, at 0.0216%. The ANOVA for cellulose content was presented in
Table 5, which was used to check the model adequacy (Lin et al., 2021). The p-value of the model was 0.0004, which was lower than
0.05, indicating the significance of the model. The p-value for the two main effects, namely PL:S and soda concentration, was also
lower than 0.05, with 0.0004 and 0.0046, respectively. Therefore, both main effects were significant. Meanwhile, the p-value for
temperature and pulping time was greater than 0.05, which was insignificant. This might be due to the range chosen for each
parameter not being significant towards the process. Equation (4) displays a model that correlates the interaction between input and
output variables, with A, B, C, and D denoting PL:S, soda concentration, temperature, and pulping time, respectively.
Cellulose content (%) = 23.9 − 1.78A + 0.8B + 0.22C − 0.15AB − 1.85AD + 1.9BC + 0.94BD + 0.081CD − 1.83ABC
+ 0.069ABD − 1.23ACD + 3.48BCD − 1.08ABC (4)
2
The equation was used to identify the interactions between all four parameters on cellulose content. The R value in the range of

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Table 5
Analysis of variance for cellulose extraction.

Source Sum of squares Mean square F value p-value

Prob > F

Model 480.46 40.04 228.28 0.0004

A-Pineapple leaf to soda ratio 50.94 50.94 290.46 0.0004
B-Soda Concentration 10.32 10.32 58.84 0.0046
C-Temperature 0.79 0.79 4.49 0.1243
D-Pulping Time 0.1 0.1 0.59 0.4973
AC 1.31 1.31 7.44 0.0721
AD 54.65 54.65 311.59 0.0004
BC 57.87 57.87 329.97 0.0004
BD 14.19 14.19 80.93 0.0029
ABC 53.62 53.62 305.71 0.0004
ACD 24.18 24.18 137.87 0.0013
BCD 193.84 193.84 1105.17 <0.0001
ABCD 18.64 18.64 106.28 0.0019

0.75–1 displays the well statistical model (Lin et al., 2021). The R2 for this model is 0.9971, suggesting a good fit to the experimental
data and could represent the process. The value implies that this mathematical model could describe the 99.71% variability in the
cellulose yield (Lin et al., 2021).
The main and interaction effects of the parameters on the cellulose content (%) were displayed by the Pareto chart in Fig. 4. The PL:
S (parameter A) was positioned above the Bonferroni line; meanwhile, soda concentration (parameter B) lies above the t-value limit
line, displaying the significance of both parameters towards the cellulose content. Temperature (parameter C) and pulping time
(parameter D) had no significant effect on cellulose content since the bar lies below the t-value limit. In addition, the cellulose content
was influenced by the interaction parameters between soda concentration, temperature, and pulping time (BCD). The cellulose content
increases with soda concentration, temperature, and pulping time. The positive effect was obtained when the parameter was pro­
portional to the response value, as indicated by the orange-colored bar. Cheng et al. (2011) stated that when 10% of sodium hydroxide
was applied, over 90% of the xylose could be extracted from solid substrates, so a high yield of cellulose could be achieved if the
alkaline concentration was high. As the temperature increases, the yield of cellulose will also increase since the high temperature could
enhance the delignification process (Cheng et al., 2011). According to Song et al. (2016), the dissolving capacity of any substance
increases with temperature increment. More lignin from the pineapple leaves was dissolved at a high temperature, increasing the
cellulose content.
Inversely, PL:S contributed negatively towards cellulose content, signified by the blue-colored bar. Song et al. (2016) mentioned
that the solid to liquid ratio (pineapple leaves to soda ratio) plays an important role in cellulose extraction. At a higher soda volume
(PL:S at 1: 10), the cellulose content was lower than at a low soda volume (PL:S at 1:5). This finding was in agreement with Potůček
et al. (2014), who studied the soda pulping of rapeseed straw. The increase in the alkaline liquor-to-straw ratio has negatively impacted
the degree of delignification. Therefore, the liquor-to-straw ratio of 5:1 was chosen as a suitable ratio for the tested rapeseed straw
instead of the 9:1 ratio.

Fig. 4. Pareto chart of the cellulose extraction process.

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3.4. Effect of independent and interactive parameters in the cellulose extraction

Fig. 5 represents the effect of the two most significant independent parameters on the cellulose extraction process. As illustrated by
the Pareto chart in Fig. 4 and the ANOVA table in Table 5, the PL:S and soda concentration were the two most significant parameters
contributing to the cellulose extraction. Fig. 5(a) shows that, at a PL:S ratio of 1:10, the cellulose content decreased to 24.19%.
However, the content could reach 38.14% when a lower ratio was applied. As mentioned earlier by Potůček et al. (2014) and Song et al.
(2016), the high soda volume in the mixture could affect the degree of delignification of the cellulose. A large amount of soda in the
mixture could degrade and dissolve the fiber in pineapple leaves more quickly, reducing the fiber content.
Fig. 5(b) shows the effect of soda concentration on cellulose content. It was observed that soda concentration had significantly
affected the cellulose content. The amount of cellulose was 20.23% at 5 wt% soda concentrations and increased to 38.14% at 10 wt%
soda concentrations. It is difficult for the soda to infiltrate the pineapple leaves and dissolve the lignin at a low soda volume, resulting
in a small amount of cellulose being extracted (Song et al., 2016). This explains the importance of soda concentration since the increase
in soda concentration caused an increase in cellulose content.
Fig. 6 displays the interaction between soda concentration and temperature and PL:S with pulping time. The value of the cellulose
content was the highest at 10 wt% soda concentration and 100 ◦ C temperatures, as shown in Fig. 6(a). At 60 ◦ C, the cellulose content
was the lowest at 10 wt% soda concentration. This might be due to the concentrated NaOH solution. However, the temperature was not

Fig. 5. Effect of significant independent parameters on cellulose content. (a) pineapple leaf to soda ratio; (b) soda concentration.

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Fig. 6. Effect of interactive parameters on cellulose content (a) soda concentration and temperature (BC); (b) PL:S and pulping time (AD).

high enough to start the delignification process, which resulted in the lowest cellulose content at 60 ◦ C. Fig. 6(b) depicts the interaction
between pulping time and PL:S, demonstrating that 75 min of pulping time with a 1:5 PL:S resulted in good performance. There was a
significant difference when 45 min of pulping time was applied. Pulping time displayed an insignificant effect as the main parameter.
However, it plays a decisive role when interacting with other parameters. The involvement of other parameters with pulping time
would increase the cellulose content.

3.5. Best condition for cellulose content and permittivity

The suggested best condition for soda pulping was validated, with the experimental value of the cellulose content obtained at
40.51%. The error was calculated with the predicted cellulose content of 39.38%, which was 2.78%. The low error value indicates that
the experimental value was reasonably close to the predicted values. The highest cellulose content obtained from the validation
experiment was 40.51%. A permittivity test was conducted on this sample, and the value obtained was 1.6626. Thus, by comparing the
permittivity value obtained in this study with readily available polypropylene capacitors (ϵr = 2.2), the developed material could store
energy suitable for capacitor applications.
The best conditions for the cellulose extraction process in this study were compatible with other research. Research by Cheng et al.
(2011) proved that at 10 wt% soda concentrations, 90% of cellulose was extracted from solid substrates. The temperature range for
chemical pulping is typically from 140 to 180 ◦ C, nevertheless, it varies depending on the raw material used (Musekiwa et al., 2020).

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An optimum temperature of 110 ◦ C was discovered by Wutisatwongkul et al. (2016) since the delignification process will slow down at
low temperatures. Too high temperatures will destroy the cellulose chain. The cellulose content was the highest recorded by Lim et al.
(2019) at 140 ◦ C and started to decline shortly after the temperature increment. A similar observation by Song et al. (2016) was also
recorded where the pulp yield substantially decreased after the pulping temperature exceeded 140 ◦ C. Li et al. (2014) also discovered
that the yields of bamboo pulp declined as the temperature increased from 140 to 170 ◦ C. Therefore, we can conclude that the cellulose
chain will be slowly destroyed at a temperature of more than 140 ◦ C, as proved by the literature.

3.6. Relationship between morphology, cellulose content, and permittivity value

Fig. 7 shows the morphology of the developed samples of the cellulose fiber in the pineapple leaf. As discussed in sections 3.2 and
3.6, run 14 shows the lowest percentage of cellulose content, which was 14.83%. While run 15, shows the highest percentage of
cellulose content, which was 39.38%. The cellulose fiber of the developed sample of run 14 was shown in Fig. 7(a) at the conditions of
1:10 PL: S, 5% soda concentration, 100 ◦ C temperature, and 75 min of pulping time. Fig. 7(b) is the image of the cellulose fiber of the
developed sample of run 15 at the condition of 1:5 PL:S, 10 wt % soda concentrations, 100 ◦ C temperature, and 75 min pulping time.
The size of the diameter, Ø of the cellulose fiber for runs 14 and 15 was 5.40 ± 1.37 μm and 4.25 ± 1.42 μm, respectively. The distance,
Δ between the cellulose fibers in runs 14 and 15 was 9.05 ± 1.67 μm and 7.35 ± 2.81 μm, respectively. From the SEM images, the
decrement in the diameter size of the cellulose fiber and the distance between the cellulose fibers was seen in runs 14 and 15. From
these results, we can conclude that the changes in diameter size and the distance between the cellulose fibers of the developed samples
were affected by the value of the cellulose content, where the values of both morphological parameters were not proportional to the
cellulose content. In addition, the increase in both morphological parameters significantly reduced the permittivity value. The large
diameter size of the cellulose fibers and the distance between cellulose fibers resulted in a low permittivity value (Jabal et al., 2016).

4. Conclusion
This study focused on the effect of processing parameters on cellulose extraction and the determination of the most significant
parameter in the cellulose extraction process. The study showed that PL:S was the most significant parameter, with the highest per­
centage contribution. The best conditions for the cellulose extraction process obtained from TLFA were at 1:5 PL:S, 10 wt% soda
concentration, 100 ◦ C temperature, and 75 min of pulping time. At this condition, the cellulose content was up to 40.51%, with a
1.6626 permittivity value. By comparing the cellulose content values from OFAT and TLFA, it can be concluded that detailed analysis
in TLFA could improve the cellulose yield, increasing its corresponding permittivity value. The findings of this study can contribute
significantly to future studies on the optimization of processing parameters for optimum extraction conditions. It is also recommended
to investigate the effects of other parameters on the cellulose extraction process in OFAT analysis since this research only analyzes the
effect of pulping time on cellulose extraction to further understand the behavioral pattern of each processing parameter.

Funding
This work was supported by Universiti Malaysia Pahang and the Ministry of Education under the Fundamental Research Grant
Scheme (FRGS) with reference no. FRGS/1/2018/STG02/UMP/02/1. This work was also partly supported by the Research and
Innovation Department, Universiti Malaysia Pahang, under a research grant with reference no. RDU1903131.

CRediT authorship contribution statement

M.S. Abdul Karim: Methodology, Resources, Supervision, Project administration, Conceptualization. N. Zainol: Methodology,
Data curation, Supervision, Funding acquisition, Project administration, Conceptualization. N.I.A. Abu Hassan As’ari: Writing –

Fig. 7. SEM image of cellulose fiber of pineapple leaf; (a) run 14 of the developed sample; (b) run 15 of the developed sample.

10
M.S. Abdul Karim et al. Biocatalysis and Agricultural Biotechnology 42 (2022) 102339

original draft, Preparation. N. Abu Talip Yusof: Methodology, Investigation, Writing – original draft, Preparation. N.H. Aziz: Writing
– review & editing.

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.

Acknowledgment
The authors would like to extend their gratitude to Universiti Malaysia Pahang and the Ministry of Education (MoE) for the
approved fund making this research possible.

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