Carbohydrate Polymers 181 (2018) 1038–1051

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Carbohydrate Polymers
journal homepage: www.elsevier.com/locate/carbpol

Research paper

Isolation and characterization of nanocrystalline cellulose from sugar palm T

fibres (Arenga Pinnata)
⁎
R.A. Ilyasa, S.M. Sapuana,b, , M.R. Ishakc
a
Laboratory of Biocomposite Technology, Institute of Tropical Forestry and Forest Products, Universiti Putra Malaysia, 43400 UPM, Serdang, Selangor, Malaysia
b
Department of Mechanical and Manufacturing Engineering, Universiti Putra Malaysia, 43400 UPM, Serdang, Selangor, Malaysia
c
Department of Aerospace Engineering, Universiti Putra Malaysia, 43400 UPM, Serdang, Selangor, Malaysia

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

Keywords: Cellulose was extracted from sugar palm fibres (Arenga pinnata) by conducting delignification and mercerization
Sugar palm fibres treatments. Subsequently, sugar palm nanocrystalline celluloses (SPNCCs) were isolated from the extracted
Cellulose cellulose with 60 wt% concentrated sulphuric acid. The chemical composition of sugar palm fibres were de-
Sugar palm nanocrystalline cellulose termined at different stages of treatment. Structural analysis was carried out by Brunauer-Emmett-Teller (BET),
Nanofibre
X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR). Morphological analysis of extracted
Thermal behavior
cellulose and isolated nanocrystalline cellulose (NCCs) was investigated by using field emission scanning elec-
Acid hydrolysis
tron microscopy (FESEM), atomic force microscopy (AFM), and transmission electron microscopy (TEM). The
thermal stability of sugar palm fibres at different stages of treatment was investigated by thermogravimetric
analysis (TGA). The results showed that lignin and hemicellulose were removed from the extracted cellulose
through the delignification and mercerization process, respectively. The isolated SPNCCs were found to have
length and diameters of 130 ± 30 nm and 9 ± 1.96 nm, respectively.

1. Introduction xylose, glucose, arabinose, mannose and galactose. However, both

Nanocrystalline celluloses (NCCs) isolated from plant fibers at-
tracted a tremendous interest in material science due to its appealing
intrinsic properties including nano-dimension, high surface area
(100 m2 g−1) (Islam, Alam, & Zoccola, 2013; Savadekar & Mhaske,
2012; Silvério, Flauzino Neto, Dantas, & Pasquini, 2013), high aspect
ratio of 100 (Rosa et al., 2010; Savadekar & Mhaske, 2012; Tee et al.,
2013a, 2013b), high crystallinity, low density, high mechanical
strength, unique morphology along with availability, renewability and
biodegrability (Azizi Samir, Alloin, & Dufresne, 2005; Ilyas, Sapuan,
Ishak, & Zainudin, 2017; Ng et al., 2015). Cellulose is the product of
biosynthesis from bacteria and plants, whereas the general term “na-
nocrystalline cellulose” refers to cellulosic isolation or extraction ma-
terials, with the outstanding feature of nano-scale structural dimension.
The main component of plant fibres is cellulose, semicrystalline
polymer, which composed of poly(1,4-β-D-anhydroglucopyranose)
units. These units are formed from strong hydrogen bond between
hydroxyl groups. Other main components that made up natural fibres
structure are lignin and hemicellulose. Lignin is a highly cross-linked
phenolic polymer, whereas hemicellulose is a branched multiple poly-
saccharide polymer composed of different types of sugars comprising
lignin and hemicellulose are amorphous polymers. Strong acid hydro-
lysis is a well-known process for the removal of the amorphous region
and isolation of NCCs from natural fibers. Under controlled conditions,
acid hydrolysis allows removal of the amorphous regions of cellulose
fibres whilst keeping the crystalline domains intact in the form of
crystalline nanoparticles. In fact, removing the amorphous region in-
fluences the structure, thermal stability, crystallinity as well as surface
morphology of the fibres (Ilyas Rushdan et al., 2017). Previous studies
done by Deepa et al. (2011a) and Li et al. (2009), have shown im-
provement in the thermal stability and crystallinity during the isolation
of NCCs.
In the past decades, many different resources have been used to
prepare NCCs, such as hard- and softwood fibres (Beck-Candanedo,
Roman, & Gray, 2005), wheat straw (Dufresne, Cavaillé, & Helbert,
1997), sisal (Garcia de Rodriguez, Thielemans, & Dufresne, 2006a;
Garcia de Rodriguez, Thielemans, & Dufresne, 2006b; Morán, Alvarez,
Cyras, & Vázquez, 2008), pineapple leaves (Cherian et al., 2010a), co-
conut husk fibres (Rosa et al., 2010), mulberry (Li et al., 2009), bananas
(Deepa et al., 2011a), sugarcane bagasse (de Morais Teixeira et al.,
2011), bamboo (Brito, Pereira, Putaux, & Jean, 2012), mengkuang
leaves (Sheltami, Abdullah, Ahmad, Dufresne, & Kargarzadeh, 2012),

⁎
Corresponding author.
E-mail address: sapuan@upm.edu.my (S.M. Sapuan).

https://doi.org/10.1016/j.carbpol.2017.11.045
Received 8 June 2017; Received in revised form 25 October 2017; Accepted 14 November 2017
Available online 15 November 2017
0144-8617/ © 2017 Published by Elsevier Ltd.
R.A. Ilyas et al.
jute (Cao, Ding, Yu, & Al-Deyab, 2012), rice straw (Lu & Hsieh, 2012),
eucalyptus wood (Tonoli et al., 2012), soy hull (Flauzino Neto, Silvério,
Dantas, & Pasquini, 2013), cotton linter (Morais et al., 2013) and kenaf
bast (Zaini, Jonoobi, Tahir, & Karimi, 2013). The purpose of the iso-
lation of NCCs is as reinforcements in the field of nanocomposite that
has gained tremendous attention since it was first examined by Favier
et al. (1995). However, no studies on the production, composition, or
properties of natural nanocrystalline cellulose fibres from sugar palm
fibres have been found in the literature.
Sugar palm tree also known as Arenga Pinnata is a popular multi-
purpose tree dominantly found in tropical regions. It belongs to the
Palmae family which has about 181 genera with around 2600 known
species (Ishak et al., 2013). The fruit can be eaten as sweet meal and the
fibres can be used for weaving hat and mats, making ropes, brooms,
road construction, brushes, roof materials, cushion and shelters for fish
breeding. Besides that, its stem core can be used for making sago flour
and root as tea to cure bladder stones; insect repellent and posts for
pepper, boards, tool handles, water pipes, musical instruments like
drums (Adawiyah, Sasaki, & Kohyama, 2013; Ishak et al., 2013; Martini
et al., 2012; Mogea, Seibert, & Smits, 1991). Up to the present time, the
usage of sugar palm fibres has progressed to another successive level
especially to numerous engineering applications. In example, it is being
used for underground and underwater cables, substitution of geo-textile
fiberglass reinforcement in road construction for soil stabilization as
well as a used as reinforcement in polymer matrix composite in material
engineering (Ishak et al., 2013). Several studies have shown that sugar
palm fibres have a huge potential to be used in various polymer com-
posite application (Bachtiar, Sapuan, & Hamdan, 2008, Bachtiar,
Sapuan, & Hamdan, 2010, Bachtiar, Salit, Zainudin, Abdan, & Dahlan,
2011; Ishak, Leman, Sapuan, Salleh, & Misri, 2009; Sahari, Sapuan,
Ismarrubie, & Rahman, 2011, Sahari, Sapuan, Zainudin, & Maleque,
2013a, Sahari, Sapuan, Zainudin, & Maleque, 2013b). This study con-
tinues with sugar palm-derived cellulose reinforced with starch
polymer (Sanyang, Sapuan, Jawaid, Ishak, & Sahari, 2016). To the best
of our knowledge, no study on sugar palm nanocrystalline cellulose
(SPNCCs) has been found in the literature. Thus the aim of the current
study was to extract and characterize nanocrystalline cellulose (NCCs)
from sugar palm fibres.
In this paper, cellulose and NCCs were extracted from sugar palm
fibres by chemical and mechanical methods. The effects of different
chemical treatments on sugar palm fibres were investigated by de-
termining their chemical composition (TAPPI standard), thermogravi-
metric analysis (TGA), X-ray diffraction (XRD), surface area by
Brunauer-Emmett-Teller (BET), degree of polymerization (DP), Fourier
transform infrared (FT-IR) spectroscopy and field emission scanning
electron microscopy (FESEM). The aspect ratio and dimensions of the
isolated NCCs were determined by using zeta potential nanoparticle
sizer, atomic force microscopy (AFM) and transmission electron mi-
croscopy (TEM).
2. Experimental
2.1. Materials
Sugar palm fibres gathered in Bahau (Negeri Sembilan, Malaysia)
were used in this study. The chemical reagents used were sodium
chlorite, acetic acid, sodium hydroxide and sulphuric acid (purchased
from Sigma–Aldrich).
2.2. Extraction of cellulose
Cellulose fibres can be extracted from sugar palm fibres (SPF) using
two main processes, which are delignification and mercerization (Ilyas
et al., 2017; Sanyang et al., 2016; Tawakkal, Talib, Abdan, & Ling,
2012; Tee et al., 2013a, 2013b). The initial process was performed in
accordance with ASTM D1104-56 (1978) to prepare holocellulose
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Carbohydrate Polymers 181 (2018) 1038–1051
through a chlorination or bleaching process, primarily designed for the
removal of lignin from SPF. 20 g of SPF was rinsed with tap water to
remove foreign particle and dust. The clean SPF then soaked in a
1000 mL beaker containing 650 mL of hot distilled water with tem-
perature of 95 °C, which then was transferred to a water bath, and the
temperature was set at 70 °C. 4 mL of acetic acid and 8 g of sodium
chlorite was added to the beaker every hour for 7 h, consecutively. The
changing color of the SPF from light brown to white indicated the level
of delignification. The obtained celluloses are referred to as holocellu-
lose and were filtered, washed and rinsed with distilled water.
The holocellulose were further treated to produce α-cellulose ac-
cording to ASTM D1103-60 (1977). The holocellulose were then soaked
in 500 mL of 5% w/v NaOH solution for 2 h at 23 ± 2 °C. The cellulose
produced were filtered and immerged in 500 mL of distilled water
containing approximately 7 mL of acetic acid to neutralize the cellulose.
Then, the mixture was stirred for approximately 30 s before it was al-
lowed to settle for 5 min. It is then rinsed with water until the cellulose
residue was free from acid as indicated by a pH meter. Lastly, the cel-
lulose denoted as sugar palm cellulose (SPC) was dried in an oven at
103 °C overnight.
2.3. Isolation of sugar palm nanocrystalline cellulose (SPNCCs)
SPNCCs were prepared by acid hydrolysis of the cellulose obtained
as described elsewhere (Sanyang et al., 2016). Acid hydrolysis was
carried out using 60 wt% H2SO4 solution and kept stirring with me-
chanical stirrer 1200 rpm for 45 min at 45 °C. The time of hydrolysis in
this study was fixed at 45 min, which was found to be the optimum time
(Bondeson, Mathew, & Oksman, 2006a). The ratio of the obtained
cellulose to liquor was 5:100 (wt%) (5 g cellulose: 100 g H2SO4 solu-
tion). The hydrolyzed cellulose samples were washed four times by
centrifugation (6000 rpm, 20 min, and 10 °C) to eliminate the leftover
sulphuric acid. The suspension was then dialyzed against distilled water
until a constant pH was reached (6.5–7). Then, the resultant suspension
was sonicated for 30 min. Lastly, the suspension was freeze-dried at
−110 °C using ethylene gas and stored at cool place prior to sample
analysis (Bondeson et al., 2006a; Sheltami et al., 2012).
2.4. Characterization
2.4.1. Determination of chemical composition
The chemical compositions of sugar palm fibres were determined at
different stages of treatment such as raw fibres, bleached fibres and
alkali-treated fibres. The percentage of holocellulose was determined
according to the method described by Wise, Murphy, and D’Addieco
(1946). Determination of lignin (acid insoluble) and α-cellulose and
contents were determined according to TAPPI standard methods T 222
(acid-insoluble lignin in wood and pulp) and T 203 (alpha-, beta- and
gamma-cellulose in pulp), respectively. It should be noted that the
procedure used for this standard has been modified by the Institute Of
Tropical Forestry And Forest Products, Universiti Putra Malaysia (IN-
TROP-UPM).
2.4.2. Field emission scanning electron microscopy (FESEM)
Field emission scanning electron microscopy (FESEM) micrographs
were taken using an FEI NOVA NanoSEM 230 machine with an accel-
erating voltage of 3 kV to observe the micro and nanostructure surface
of the longitudinal cross section of dried sugar palm fibres, as well as
the fibres after different stages of treatment and SPNCCs. Besides, to
avoid over charging, all samples were coated with gold (Hajalilou,
Hashim, & Mohamed Kamari, 2014; Sheltami et al., 2012).
2.4.3. Transmission electron microscopy (TEM)
The transmission electron microscopy (TEM) machines are used to
produce nanostructure images of the SPNCCs. The Philips Technai 20
machine with acceleration voltage of 200 kV and standard inclined
R.A. Ilyas et al.
sample holder produces the TEM images was used. Firstly, a suspension
of SPNCCs were dispersed by ultrasonicating apatite particles in dis-
tilled water for 10 min. After that, one drop of a diluted suspension of
SPNCCs were placed on a carbon coated copper grid, then allowed to
dry at room temperature. The TEM nanostructures images were en-
hanced to improve the resolutions (Hofmeister & Platen, 1992).
2.4.4. Density
The density was measured using gas intrusion under a helium gas
flow with an AccuPyc 1340 pycnometer. The samples are being oven
dry at 105 °C overnight to remove moisture content within the fibres.
After that the samples were place inside the desiccator to remove traces
of water from almost-dry sample before placed inside the pycnometer.
Five measurements were conducted at 27 °C and the average value was
computed (Jumaidin, Sapuan, Jawaid, Ishak, & Sahari, 2017a;
Jumaidin, Sapuan, Jawaid, Ishak, & Sahari, 2017b, Jumaidin, Sapuan,
Jawaid, Ishak, & Sahari, 2017c).
2.4.5. Moisture content
Five samples were prepared for the moisture content investigation.
All samples were heated in an oven for 24 h at 105 °C. Weight of
samples before, Mi and after, Mf the heating were measured in order to
calculate the moisture content (Jumaidin et al., 2017a, 2017b, 2017c).
Moisture content was determined by using Eq. (1).
Mi − Mf
Moisture content = × 100
Mi (1)
2.4.6. Yield
Yield was calculated as percentage, % of initial weight of sugar palm
cellulose (SPC) after hydrolysis. The suspension of the SPNCCs gained
after dialysis treatment was freeze-dried and compare to the initial
weight of SPC. Weight of samples final of SPNCCs, Mf and initial of SPF,
Mi were measured in order to calculate the yield (Bondeson et al.,
2006a). Yield was determined by using Eq. (2).
Mf
Yield% = × 100
Mi (2)
2.4.7. Fourier transform infrared (FT-IR) spectroscopy
Fourier transform infrared (FT-IR) spectroscopy was used to detect
possible changes in the functional groups existing in sugar palm fibre at
different stages of extraction. Spectra of the material were obtained
using an IR spectrometer (Nicolet 6700 AEM). FT-IR spectra of the
samples (10 × 10 × 3 mm) was collected in the range of
4000–500 cm−1. Ground samples were mixed with KBr, after which
the mixture was pressed into thin transparent films that were analysed
(Jumaidin et al., 2017a, 2017b).
2.4.8. X-ray diffraction (XRD)
Rigaku D/max 2500 X-ray powder diffractometer (Rigaku, Tokyo,
Japan) equipped with CuKα radiation (λ = 0.1541 nm) in the 2θ range
10–40° was used to study X-ray diffraction patterns of the raw,
bleached, alkali-treated fibres and hydrolysis of sugar palm fibres. Then
empirical method (Segal, Creely, Martin, & Conrad, 1959) was used to
obtain the crystallinity index of the samples Xc, as shown in Eq. (3):
I002 − Iam
Xc = × 100
I002 (3)
where I002 and Iam are the peak intensities of crystalline and amorphous
materials, respectively.
2.4.9. Zeta potential
The zeta potential measurements were performed using a Zetasizer
Nano-ZS (Malvern Instruments, Worcestershire, UK) to determine the
approximate size of SPNCCs and to characterize the surface charge
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Carbohydrate Polymers 181 (2018) 1038–1051
property of nanoparticles. A tenfold dilution of the samples in pure
water in a total volume of 1 mL was subjected to a particle size analyzer
at 25 °C. The measurement was based on the electrophoretic mobility
(μm/s) of the particles which was converted to zeta potential by inbuilt
software based on the Helmholtz–Smoluchowski equation (Morais
et al., 2013).
2.4.10. Thermogravimetric analysis (TGA)
The thermal degradation behaviour of composites was analyzed by
TGA with respect to weight loss due to increase in temperature. TGA
was performed with a Q series thermal analysis machine from TA
Instruments (New Castle, DE, USA) to determine the thermal stability of
sugar palm fibres at different stages of extraction. The analysis was
carried out in aluminum pans under a dynamic nitrogen atmosphere in
temperature range 25–600 °C at a heating rate of 10 °C/min−1
(Jumaidin et al., 2017a, 2017b).
2.4.11. Surface area and porosity measurements
The surface areas, pore sizes and pore size distribution were mea-
sured by Brunauer-Emmett-Teller (BET) method or N2 adsorption-
desorption at 77 K by using a surface area and porosity analyszer
BELSorp Mini II (NIKKISO, Osaka, Japan). The samples were degassed
at 105 °C under vacuum for 10 h. Specific surface areas were derived
from the linear region of the isotherms using the Brunauer-Emmett-
Teller (BET) equation in a relative P/Po pressure range 10-2 to 1,
whereas pore size distribution were calculated from adsorption branch
of the isotherms by Barrett-Joyner-Halenda (BJH) method. The total
pore volumes were estimated from the amount absorbed at a relative
pressure of P/Po = 0.98.
2.4.12. Atomic force microscopy (AFM)
The AFM measurement were conducted using Dimension Edge with
High-Performance AFM (Bruker, Santa Barbara, CA, USA) equipment
and Bruker Nanoscope analysis software (Version 1.7) operated using
Peak/Force tapping mode with one controller (Nanoscope V from
Bruker) for evaluating the evaluating the thickness of the SPNCCs.
Initially, a drop of diluted SPNCCs aqueous suspension was deposited
on the surface of an optical glass slide and allowed to air dry. The
SPNCCs were scanned in air at room temperature of 25 oC and relative
humidity in tapping mode with OMCL-AC160TS standard Si probes (tip
radius < 10 nm, spring constant = 2.98 N/m, resonant
frequency = ∼310 kHz) under a 1 Hz scan rate.
2.4.13. Degree of polymerization (DP)
The degree of polymerization (DP) of SPF, SPBF, SPC and SPNCCs
fibres suspension was determined based on the intrinsic viscosity[η].
Viscosity measurement for fibres suspension was carried on according
to TAPPI Standard Method T230 om-08 and ISO 5351-1 as reported by
Chauve et al. (2013). Fibres were diluted in solutions containing dis-
tilled water and copper (II) ethylenediamine (CED) solution as dissol-
ving agent with a ratio 0.01:1:1 (treated fibre: distilled water: CED).
The solution was shaken until all the fibres were completely dissolved.
The viscosity of this solution and the solvent was measured at 25 °C
using Ubbelohde viscometer tube (Type 231, PTA Laboratory Equip-
ment, Vorchdorf, Austria). The experiment was performed for all the
samples and repeated three times. The molecular weight of treated fibre
was calculated using the Mark-Houwink approach, which was using Eq.
(4),
[η] = KMα (4)
where [η] the intrinsic viscosity and M is the molecular weight. The
values of the constants were taken as K = 0.42 and α = 1 for the CED
solvent (Ilyas et al., 2017; Yasim-Anuar, Ariffin, Norrrahim, & Hassan,
2017).
R.A. Ilyas et al.
Table 1
Chemical composition of sugar palm fibres at different stages of treatment.
Samples Cellulose (%) Hemicellulose (%)
Sugar Palm fibres 43.88 7.24
Bleached fibres 56.67 19.8
Alkali-treated fibres 82.33 3.97
3. Results and discussion
The chemical compositions of the sugar palm fibres were affected by
the chemical extraction process, NaClO2 followed by NaOH. From raw
sugar palm fibres as feedstock, the initial stage of the extraction process
was bleaching treatment. This treatment was done to remove lignin
(Dufresne, Dupeyre, & Vignon, 2000; Sheltami et al., 2012). The
bleaching treatment effects are depending on the temperature and pH.
Usually, the reaction happens at high temperature and low pH. The
second stage was alkali treatment that was done to remove and hy-
drolyze the hemicellulose, silica, soluble mineral salts, and ash (Deepa
et al., 2011b; Ndazi, Nyahumwa, & Tesha, 2007). The morphology of
the raw and treated sugar palm fibres were influenced by this alkali
treatments.
3.1. Chemical composition
The chemical compositions of the sugar palm fibres at different
stages of treatment are shown in Table 1. From Table 1, it shows that
the original sugar palm fibres consist of 43.88% cellulose, 7.24%
hemicellulose, 33.24% lignin, 2.73% extractive and 1.01% ash. After
treating the sugar palm fibres with NaClO2 solution, the cellulose
content was increased by 12.79%, whereas the lignin was reduced by
about 32.97%. Lignin was removed in large amount after 7th round of
bleaching, with duration of each round is 1 h. The usage of NaClO2 for
the 1st stage is an excellent choice for lignin removal as natural fibres
can be considered as composite of hollow cellulose fibrils collected by
lignin as binder in a hemicellulose matric. Hence, the removal of the
hemicellulose after the lignin removal would be eased. The extensive
reduction of the hemicellulose content in fibres occurred in alkali
treatment, which was reduced to 3.97% from 19.8%. Lignin was solu-
bilized by bleaching treatment, whereas dilute alkali treatment solu-
bilized the hemicellulose and remaining lignin in the fibres. This was
affected by cleavage of the ester-linked substance of hemicellulose,
where this treatment increased the surface area of the sugar palm fibres
to make polysaccharides more vulnerable to hydrolysis. Besides that, it
is clear from Table 1 that the chemical treatment removed most of the
lignin and hemicelluloses from the sugar palm fibers. The lignin content
was decreased from 33.24% to 0.06% and hemicellulose from 7.24 to
3.97% whereas α-cellulose content was increased from 43.88% to
82.33%. The changes of chemical composition of sugar palm fibres after
all treatment resulted in a better crystalline degree of cellulose and
therefore improved the strength and thermal properties of the fibers
(Alemdar & Sain, 2008).
3.2. Morphological analysis of sugar palm fibres, treated fibres and SPNCCs
3.2.1. Morphological analysis of sugar palm fibres
The bleaching and alkali treatments not only resulted in changes of
chemical composition of the treated fibres, they also affect the structure
of the fibres surfaces. Fig. 1 shows the sugar palm tree and its fibres at
different stages of treatment. The color of the sugar palm fibres changed
from black (Fig. 1d) to light brown after bleaching treatment (Fig. 1e)
and became white after alkali treatment (Fig. 1f). FESEM pictures of
sugar palm fibres were taken to investigate the structure of sugar palm
fibers to reveal their homogeneity and micrometric dimensions, and are
also shown in Fig. 1. Microscopic examination of the longitudinal and
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Carbohydrate Polymers 181 (2018) 1038–1051
Holocellulose (%) Lignin (%) Extractive (%) Ash (%)
51.12 33.24 2.73 1.01
76.47 0.27 0.23 2.16
86.3 0.06 – 0.72
cross section of sugar palm fibres was depicted in Fig. 1b,c,g. Fig. 1g
indicates sugar palm fibres (SPF) with approximate diameter size of
212.01 ± 2.17 μm, in the original form were bonded together by ce-
ment components known as middle lamella, which were partially di-
minished after the bleaching treatment (Fig. 1h). As pointed out by
Alemdar and Sain (2008) and Rosa et al., 2010 worked with wheat
straw and soy hull, and coconut fibres, respectively, these images shows
the partial removal of impurities pectin, lignin and hemicellulose after
chemical treatment, which they are acting as cementing components
surround fibre-bundles.
As seen in Fig. 1b,c, the view from the outer to the inner part
showed that sugar palm fibres consist of a middle lamella, a primary, a
secondary and a tertiary cell wall, build up around an opening, the
lumen (Bledzki & Gassan, 1999). The middle lamella as seen in Fig. 1c,
which is surround the cell wall is mainly composed of pectins (mac-
romolecules of galacturonic acid) that hold fibres together into a
bundle, with a size around 1.98 ± 0.15 μm.
The interior of the sugar palm fibres consist of primary cell wall,
secondary cell wall, and lumen. Primary cell wall is made of cellulose (a
polymer baesd on glucose units) fibrils in an organic matrix of amor-
phous hemicelluloses and lignin, proteins, and low methylesterified
pectins, with the average diameter being around 10.38 ± 0.57 μm.
The secondary cell wall consist of three layers of cellulose fibrils with
different axial orientation that are bound by lignin (Mohanty, Misra, &
Hinrichsen, 2000). Primary cell wall and secondary cell wall also pro-
vide mechanical support to the plant. Fig. 1c shows a lumen with a
thickness of around 3.72 ± 0.15 μm.
From Fig. 1 g, it can be seen that the longitudinal section of SPF
surface topography is rough, with pore-like spots that appear in almost
regular intervals, where these similar spots were also found at the
surface of coir fibres (Ticoalu, Aravinthan, & Cardona, 2013). These
pore-like spots are known as tyloses, which their function is to cover the
pits on the cell walls.
Besides that, based on the observation on sugar palm fibres micro-
structure, there is strong evidence that the acid/bleaching treatment
(NaClO2) changed the physical surface appearance of sugar palm fibres
compared to raw sugar palm fibres (Fig. 1a, h). It showed that a drastic
physical changes with slight fibrillation was clearly observed on the
outer surface of the fibres where the outer surface became clear and this
was due to the removal of the waxy layer on the outer surface. The
average diameter of bleached fibres was reduced after chemical treat-
ment from 212.01 ± 2.17 μm to 121.80 ± 10.57 μm. These were
measured after the partial removal of lignin and hemicelluloses lignin,
in another words, because of the elimination of the primary walls,
which was further supported by chemical analysis data given in
Table 1. Furthermore, the bleaching treatment removed the extractives
from the fibres indicated by the surface changing. After alkali treatment
(Fig. 1i), the fibre bundles where dispersed into individual fibres with
diameters in the range 11.87 ± 1.04 μm. Compared with raw sugar
palm fibres, bleached fibres and alkali-treated fibres was almost double
and eighteen time smaller than raw sugar palm fibres, respectively. The
removal of lignin and hemicellulose through the process of delignifi-
cation and mercerization of raw SPF had caused drastic reduction in the
diameter of bleached and alkali-treated fibres, besides the surface of
SPC (Fig. 1i) had changed to smooth and groovy surface with parallel
arrangement along the cellulose. The diameter of SPC obtained is
supported with the average diameter of kenaf-derived cellulose (13 μm)
R.A. Ilyas et al. Carbohydrate Polymers 181 (2018) 1038–1051

Fig. 1. Photographs of (a) the sugar palm tree, (d) raw sugar palm fibres, (e) bleached fibres and (f) alkali-treated fibres; FESEM micrographs of sugar plant fibres: (g) cross section, (b)
longitudinal section, (c) primary, secondary cell wall and middle lamella, (h) alkali-treated fibres, (i) and bleached fibres.

and cellulose microfibres reported by Sonia et al. (2013) and Tawakkal
et al. (2012), respectively. Besides that, similar reports have been
documented on the surface appearance of many natural fibre-derived
cellulose (Sanyang et al., 2016; Tawakkal et al., 2012; Tee et al., 2013a,
2013b). The chemical treatments used on the fibres also affected the
characterization of the separation of micro-sized fibres from the fibres
bundle into individual micro-sized fibres.
3.2.2. Isolation of SPNCCs
Delignification and mercerization resulted in partial defibrillation
and opening of fiber-bundles. Removing the cementing components and
defibrillation via bleaching-treatment and alkali treatment are im-
portant steps towards producing more efficient SPNCCs hydrolysis.
Each microfibril bundle is composed of a bundle of NCCs
interconnected along the microfibril by amorphous region (defected
structure). Under the hydrolysis process, these regions were eliminated
to yield highly NCCs, resulting in a diameter reduction and separation
of fibres from agglomerates micron-sized fibres to individual nanofibres
(Azizi Samir et al., 2005; Bondeson et al., 2006a). Usually these NCCs
range in length and diameter from 100 to 250 nm and 5–80 nm, re-
spectively, for most cellulosic material, subsequently become more or
less individualized thru sonification (Bondeson et al., 2006a).
The yield of SPNCCs was about 29% after 45 min of hydrolysis
treatment (of initial weight). The obtained yield for SPNCCs is an
agreement with the yield of sisal (30%) and mengkuang leaves (28%)
reported by Garcia de Rodriguez et al. (2006b) and Sheltami et al.
(2012), respectively. In a separate investigation, de Morais Teixeira
et al. (2011) also reported that the yield of sugarcane bagasse NCCs is

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R.A. Ilyas et al. Carbohydrate Polymers 181 (2018) 1038–1051

Fig. 2. (a) Aqueous suspension (2 wt%), (b) FESEM micrograph, (c) height measurement of NCCs using atomic force microscopy (AFM), (d) transmission electron (TEM) micrograph, (e)
atomic force microscopy (AFM) and their length (f and h) and diameter (g and i) histograms of nanocrystalline cellulose extracted from sugar palm fibres.

58%, which was twice higher than that the yield SPNCCs. The differ-
ences of the yield gained is depending on the source sample, pretreat-
ment and hydrolysis condition (Eichhorn et al., 2010; Ng et al., 2015).
It is well known that the advantage of using sulphuric acid for hydro-
lysis treatment is, this chemical contribute to the isolated crystalline
particle and stable aqueous suspensions of NCCs, due to negatively
charged, hence do not tend to agglomerate. In more detail, these
charged induce electrostatic repulsion forces between nanoparticles,
thus lead to a stable suspension (Bondeson, Mathew, & Oksman, 2006b;
Samir, Alloin, Paillet, & Dufresne, 2004). This may be attributed to the
process of esterification on the surface of hydroxyl groups from cellu-
lose during hydrolysis process, and as a consequence, the sulphate

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R.A. Ilyas et al. Carbohydrate Polymers 181 (2018) 1038–1051

groups are introduced in the outer surface of NCCs (Habibi, Lucia, &
Rojas, 2010). Moreover, the presence of sulphate group also has been
verified to decrease the material thermal stability (Roman & Winter,
2004a). Hence, all these properties are the important key factor when
NCCs are incorporated as nanoreinforcement within nanocomposite.
The resultant suspension of isolated SPNCCs prepared from cellulose
sugar palm fibre is shown in Fig. 2a. The concentration of this sus-
pension was 2 wt%. FESEM, TEM and AFM observation and the dis-
tribution of length and diameter of SPNCCs are shown in Fig. 2b–i,
respectively. The SPNCCs were characterized and analyzed by particle
length (L), diameter (D) and aspect ratio (L/D). The diameters and
length of the fibers after hydrolysis treatments were calculated by an
image processing analysis program, Image J, using the FESEM, TEM
and AFM images. The profile analysis was carried out with peak fitting
program using Gaussian line shape to define the average diameter and
length of SPNCCs. Sugar palm NCCs ranged in length from 45 to
238 nm, with an average value around 130 ± 30.23 nm. The diameter
was in the range 3–18.19 nm, with an average value around
9 ± 1.96 nm. The diameter measured were similar to the nano-sized
structures that were extracted from other agro-residue sources such as
coconut husk (5.5 ± 1.5 nm) (Rosa et al., 2010), rice straw (5.06 nm)
(Thiripura Sundari & Ramesh, 2012), soy hulls (4.43 ± 1.20 nm)
(Flauzino Neto et al., 2013), sugarcane bagasse (4 ± 2 nm) (de Morais
Teixeira et al., 2011), banana residues (5 nm) (Zuluaga, Putaux,
Restrepo, Mondragon, & Gañán, 2007) and smaller than microfibrils
from wheat straw (10–80 nm) (Alemdar & Sain, 2008), sisal fibres
(30.9 ± 12.5 nm) (Morán et al., 2008) and sugarcane bagasse (30 nm)
(Bhattacharya, Germinario, & Winter, 2008) as shown in Table 2. These
resultant images revealed the efficiency used of the acid hydrolysis
treatment on sugar palm fibres and endorsed that the aqueous sus-
pensions contained sugar palm NCCs residing mostly of individual
crystal and some aggregates.
The optimum aspect ratios (length to diameter) of sugar palm NCCs
was calculated to be 14. The aspect ratios of sugar palm NCCs are not as
much different from each other as their actual dimensions, but quite
low compared to the value of those reported on NCCs from other cel-
lulosic sources, such as sisal (60) (Garcia de Rodriguez et al., 2006a),
cotton (15) (Qi, Cai, Zhang, & Kuga, 2009), wood (35–38)(Roman &
Gray, 2005), ramie (25–42)(Habibi et al., 2008), sisal (43) (Siqueira,
Bras, & Dufresne, 2010), and tunicate (251–493)(Iwamoto, Kai, Isogai,
& Iwata, 2009).
Correspondingly to the TEM sample preparation, the AFM sample
preparation can also cause the nanocrystalline cellulose to aggregate in
their images. However the AFM analysis allows the discernment of in-
dividual NCCs of agglomerated structure through transverse height
profile. Moreover the detailed structure, topography, thickness and
roughness of the NCCs also could gained from the AFM for the purpose
of NCCs manufacturing process or functional application developer
(Flauzino Neto et al., 2013). The ultrafine fibres of SPNCCs were ex-
amined by an AFM scanning probe microscope that used only moderate
mechanical force and does not required sputter coating. According to
Azizi Samir et al. (2005), the function of the sulphuric acid hydrolysis is
to cleave the amorphous region of microfibrils transversely, which re-
sultant in reduction of the fibres diameter from micro to nanometers.
Fig. 2e shows the AFM image of sugar palm nanocrystalline cellulose
(SPNCCs) prepared by the treatment of sugar palm cellulose fibres with
sulphuric acid solution, signifying the dominant diameter ranged size of
SPNCCs was 10.7 nm ± 2.34 nm, which is similar to those obtained
from wood pulp, cotton and tunicin, probably because of the aggrega-
tion of monocrystals. These images also displayed needle-like nano-
particle. Besides, Fig. 2e also indicated the larger fibre width is due to
the tip coardening effect, which was common in AFM (Goetz, Foston,
Mathew, Oksman, & Ragauskas, 2010; Lu & Hsieh, 2012). The AFM
phase image (Fig. 2c) showed a peak nanofibres height of 5.781 nm,
comparable to the average nanofibres diameter (10.7 ± 2.34 nm) de-
termined from the AFM images. Fig. 2(g,i) shows the histograms cor-
responding to these measurements. The AFM image also showed that
the length of the SPNCCs after the sulphuric acid hydrolysis, was
around 130 ± 16.87 nm. Besides, these fibre height and width value
gained from the analysis confirmed the essentially cylindrical cross-
sectional shape of SPNCCs self-assemble fibres. The average value of
aspect ratio obtained by AFM measurements was 13, which lies in the
range of long nanocrystalline cellulose which have great potential to be
used as reinforcing agents in nanocomposites (Rosa et al., 2010).
3.3. Physical properties
One of the most important characteristics that must be considered
for a new natural materials as potential filler, especially for polymer
composite, is moisture content. Therefore, it is an important parameter
used to determine the properties and the end uses of the fibres. Low
moisture content is required, as high moisture content of the fibres
could weaken the stability of the polymer composites in terms of por-
osity formation, dimensions, and tensile strength (Jumaidin et al.,
2017a, 2017b, 2017c; Razali, Salit, Jawaid, Ishak, & Lazim, 2015). This
can be explained with the some alkali labile linkages (ester linkages and
ether linkage) between lignin and polysaccharides that were broken
during the alkali treatment, which leaving a rigid structure (cellulose)
that was durable to dissolve in the acidic solution. Therefore, as the
percentage of the cellulose content in the fibres increased, the moisture
absorption rate also increased. This is due to the chemical structure of
cellulose itself, which composed of hydroxyl groups that are accessible

Table 2
Physical properties of Sugar Palm fibres, bleached fibres, alkali-treated fibres, SPNCCs and other materials.

Samples Diameter Density (g/cm−3) Moisture content (wt Xc (%) Surface area Pore volume DP Mw (g/mol) Reference
%) (m2/g) (cm3/g)

Sugar Palm fibres 212.01 ± 2.17 μm 1.50 8.36 ± 0.0984 55.8 7.58 0.0607 – – Current study
Bleached fibres 94.49 ± 0.03 μm 1.30 ± 0.0023 6.25 ± 0.0745 65.9 10.35 0.0678 2963.33 480,513.39 Current study
Alkali-treated 11.87 ± 1.04 μm 1.28 ± 0.0019 3.83 ± 0.1037 76.0 13.18 0.1950 946.48 153,458.51 Current study
fibres
Sugar Palm NCC 9 ± 1.96 nm 1.05 ± 0.0023 17.901 ± 0.0623 85.9 14.47 0.2260 142.86 23,164.7 Current study
Coconut Husk 5.5 ± 1.5 nm – – – – – – – Rosa et al. (2010)
NCC
Rice Straw NCC 5.06 nm – – – – – – – Thiripura Sundari and
Ramesh (2012)
Sisal Fibre NCC 30.9 ± 12.5 nm – – 75.0 – – – – Morán et al. (2008)
Soy Hulls NCC 4.43 ± 1.20 nm – – 69.6 – – – – Flauzino Neto et al.
(2013)
Sugarcane 4 ± 2 nm – – 87.5 – – – – de Morais Teixeira
bagasse NCC et al. (2011)

Results expressed as mean ± standard deviation.

1044
R.A. Ilyas et al.
to water. Therefore, as related to the bleaching, alkali and hydrolysis
treatment conducted on the fibres, the fibres surface were induced to
the abundant formation of hydrophilic ionic groups, which indirectly
stimulate the absorption of moisture. As a result, we can see the in-
crement of the percentage of moisture content from raw fibres
(8.36 ± 0.0984%) to SPNCCs (17.901 ± 0.0623%).
Besides that, in material selection process, material weight is one of
the crucial parameter that have to be considered as it may affect the
performance of the products. Moreover, the main criteria that corre-
lated to this material selection properties is density. The density value
of raw sugar palm fibre, bleached-treated, alkali-treated and hydrolysis
fibres showed a decreasing value throughout the treatment, which were
1.50, 1.30 ± 0.0023, 1.28 ± 0.0019 and 1.05 ± 0.0023 g/cm−3,
respectively. This decreasing trend might be attributed to the removal
of main component of the fibres such as lignin and hemicellulose from
the fibres, the density of the fibres decreased, as shown in Table 2. The
removal of an amorphous non-cellulosic compounds component in
bleaching and alkali treatment created voids in the structure of fibres,
led swelling of fibres to occur. The constituent of fibres then became
well separated. The increasing in volume with loss in weight caused
density value to decrease (Ray & Sarkar, 2001). Besides that, the den-
sity values of SPNCCs were lower compared to conventional manmade
fibres such as glass fibre (2.5 g/cm3), aramid (1.4 g/cm3) and carbon
(1.7 g/cm3) (Mohanty et al., 2000).
Moreover, fibre density is also related to the surface area and the
porosity of fibres. The density of the fibre decrease as the pore volume
of the fibre increase. The surface areas and porosities of the macro fi-
bres and self-assembled nanofibres were determined by N2 adsorption-
desorption method 77 K. Fibres from all treatment exhibited type IV
isotherms accompanied by hysteresis loop, which is associated with
capillary condensation taking place in mesopores (2–50 nm). It is also
represent the limiting uptake over a range of high P/Po. Moreover,
these nanofibres shows an increment in cumulative pore volumes, i.e.,
0.061 cm3/g for SPF, 0.067 cm3/g for SPBF, 0.195 cm3/g for SPC and
0.226 cm3/g for SPNCCs. The cumulative pore volume for nanocrys-
talline cellulose (0.226 cm3/g) is 4 times larger than that for the raw
sugar palm fibres (0.061 cm3/g). The smaller cumulative pore volume
of the raw sugar palm fibres was expected with the rigid, closely aligned
and tightly bound building elements via strongly hydrogen bonded
cellulose structures, thus leaving little interfacial spaces (Lu & Hsieh,
2012). The result of low pore volume was confirmed by the FESEM,
TEM and AFM observation (Figs. 1 and 2). However, the pore volume of
nanocrcystalline cellulose increased after loosely packed structures took
shape to create a huge amount of mesopores among the SPNCC. The
similar trend was observed with The Brunauer-Emmett-Teller (BET)
surface area for SPF (7.578 m2/g), SPBF (10.351 m2/g), SPC
(13.1815 m2/g) and SPNCCs (14.474 m2/g). The Brunauer-Emmett-
Teller (BET) surface area of nanosize fibres from SPNCCs is 14.474 m2/
g, 2 times of those from SPF (7.578 m2/g). The higher specific surface
area of the nanofibres assembled from SPNCCs is mainly due to the
smaller fibres sizes than that of SPF.
Degree of polymerization (DP) is a crucial parameter for evaluating
the length and branching of cellulose chains, besides, to evaluate the
influence of hydrolysis in the cellulose chains that are present in na-
nocellulose. Besides that, it has been stated by Frenot et al. (2007), that
DP and molecular weight may affect the properties of cellulose such as
spinnability, solubility, and the mechanical properties of cellulose
based materials. The degree of polymerization and viscosity-average
molecular weight of the treated fibres were determined using an in-
trinsic viscosity measurement. Table 2 gives the DP value for the var-
ious treated fibres prepared in this study. The degree of polymerization
of the SPBF, SPC and SPNCCs were 2963.33, 946.48 and 142.86, re-
spectively, and the molecular weight were 480,513.39 g/mol,
153,458.51 g/mol, and 23,164.7 g/mol, respectively.
From the same table, it can be seen that the DP obtained for the SPC
was almost similar to the DP of bamboo cellulose (891) (Wang et al.,
1045
Carbohydrate Polymers 181 (2018) 1038–1051
2010), curaua cellulose (989) (Corrêa, de Morais Teixeira, Pessan, &
Mattoso, 2010), oil palm cellulose (967) (Yasim-Anuar et al., 2017).
According to Yasim-Anuar et al. (2017) the molecular weight and de-
gree of polymerization of bio-cellulose based material were ranged
from approximately 90,000 to 300,000 g/mol and 400–3000, respec-
tively. The sugar palm cellulose were in the range of the cellulose DP,
thus in good agreement with those reported in the literature.
Besides, it has been reported by Kumar et al. (2009), that deligni-
fication by the acid-chlorite process has a significant effect on the cel-
lulose chain, in which it causes a huge reduction in the average degree
of polymerization of treated fibres. Extensive delignification of SPBF
process reduced the DP to 2963, and further mercerization and hy-
drolysis process caused the DP to decrease to 946.48 and 142.86 (re-
duction percentage of 95.18%), respectively. The decreasing trend ob-
served for the DP of SPBF, SPC and SPNCCs was attributed by the
removal of lignin, hemicellulose, and amorphous region via the de-
lignification, mercerization, and hydrolysis of the raw SPF, where the
SPF bundle, SPBF and SPC fibres was cleaved and nanocrystalline cel-
lulose were released (Talib, Tawakkal, & Khalina, 2011). Moreover, the
DP reduction of cellulose was also due to the acid catalysed cleavage
during acid-chlorite delignification (Hubbell & Ragauskas 2010). Be-
sides, mercerization treatment promotes more reactive sites on the
cellulose surface (Corrêa et al., 2010). Thus, this caused acid hydrolysis
treatment to be more effective, which led to major level of breaking the
cellulose chains. According to Pääkkö et al. (2008) and Corrêa et al.
(2010), the sulphate group of strong acid leads to an extensive hydro-
lysis of amorphous phase and catalyse the degradation of the cellulose
chain, subsequently reduce DP. DP obtained for the SPNCCs was almost
similar to the DP of curaua nanofibre (101.6) (Corrêa et al., 2010) and
sugar beet pulp (120) (Habibi & Vignon, 2008).
3.4. FTIR spectroscopy analysis
Different stages of treatment on the polysaccharides (hemicelluloses
and cellulose) and lignin of sugar palm fibres were examined using FT-
IR spectroscopy. The fingerprints of the functional groups obtained for
sugar palm fibres at different stages of treatment (bleaching, alkali-
treatments and hydrolysis) are labelled in Fig. 3. The band located at
1719 cm−1 in the spectrum of raw sugar palm is attributed to C]O
stretching of the acetyl and uronic ester groups of hemicellulose or the
ester linkage of carboxylic groups of ferulic and p-coumaric acids of
lignin and/or xylan in hemicellulose (Alemdar & Sain, 2008; Fabiyi &
Ogunleye, 2015; Sun, Xu, Sun, Fowler, & Baird, 2005). This band was
d
c
b
1507
a 1593 1160
897
1227
3282
2897
1656 1316 1030
1370
1719
1424
4000 3500 3000 2500 2000 1500 1000
Fig. 3. FTIR spectra of (a) sugar palm fibres, (b) bleached fibres, (c) alkali-treated fibres,
and (d) SPNCCs.
R.A. Ilyas et al. Carbohydrate Polymers 181 (2018) 1038–1051

still present in the FT-IR of fibres after bleaching treatment and no

longer present in the FT-IR spectra of fibres after alkali and hydrolysis
treatment. The disappearance of this band could have been caused by
the removal of hemicellulose and lignin from sugar palm fibres during 800 d
the chemical extraction (Alemdar & Sain, 2008; Jonoobi, Harun,
Shakeri, Misra, & Oksmand, 2009; Sheltami et al., 2012). This was a
supported by the results obtained from determination of the chemical 600
composition of the fibres (Section 3.1 and Table 1), in which they in-
dicated that lignin was almost completely removed after the bleaching
b
treatment. However, hemicellulose was not completely removed after 400
the bleaching treatment and it was still remained after the alkali-
treatment. For this reason, the disappearance of the C = O stretching
c
band from the spectrum could be caused by cleavage of all ester-linked
200
substances of the hemicellulose by alkali treatment. Ether bonds be-
tween lignin and hemicellulose were not affected by this treatment
(Sheltami et al., 2012; Xiao, Sun, & Sun, 2001).
0
The peaks in the 1520–1510 cm−1 are determined as aromatic
5 10 15 20 25 30 35
skeletal vibration of the functional group of lignin and lignocellulose.
The band observed at 1227 cm−1, 1507 cm−1 and 1593 cm−1 are
corresponds to lignin (Faix, Lin, & Dence, 1992; Jane, Arya, & Ward, Fig. 4. X-ray diffraction patterns of (a) sugar palm fibres, (b) bleaching fibres, (c) alkali-
2012). These peak ceased after the bleaching treatment, suggesting that treated fibres, and (d) SPNCCs.
this treatment was effectively remove lignin from the fibres. These re-
sults were supported by determination of the chemical composition of
than untreated sugar palm fibres. Crystallinity degree in the structure of
the fibres as shown in Table 1. Besides, the peaks at 1475–1600 cm−1
the fibers can be identified by observing at the sharpness of the dif-
signify the structural polymer of stretching of the aromatic groups
fraction peak. The sharper the diffraction peak, the higher the crystal-
present in form of lignin (Himmelsbach, Khalili, & Akin, 2002; Sahari,
linity degree of the fibres (Alemdar & Sain, 2008). The crystallinity
Sapuan, Ismarrubie, & Rahman, 2012).
indices of raw sugar palm fibre, bleached fibres, alkali-treated fibres
Based on Fig. 3 also, the absorbance peaked in the region between
and SPNCCs were found to be 55.8%, 65.9%, 76.5% and 85.9%, re-
1630 and 1650 cm−1 and around 2900 cm−1 that reflected the
spectively. These results clearly demonstrated that the crystallinity of
stretching of the OeH and CeH groups, respectively. The peaks in the
the material progressively increases. The higher crystallinity value of
3700–3100 cm−1 region were assigned to the adsorbed water. The
SPNCCs compared to sugar palm fibres can be well understood by the
absorbance bands around 897, 1030, 1160, 1316, 1370 and 1424 cm−1
reduction and removal of amorphous non-cellulosic compounds, such
were associated with the CeH rocking vibrations, CeO stretching,
as lignin and hemicellulose induced by the bleaching, alkali and hy-
CeOeC asymmetric valence vibration, CeH2 rocking vibration and
drolysis treatments conducted in the purification process. The crystal-
CeH2 deformation vibration, respectively, where these peaks are re-
linity index of the sample after hydrolysis treatment, SPNCCs was
ferred to cellulose form of the carbohydrates (Alemdar & Sain, 2008;
higher than pineapple leaves 54% (Cherian et al., 2010b), soy hulls
Fan, Dai, & Huang, 2012; Sheltami et al., 2012). These different bands
73.5% (Flauzino Neto et al., 2013) and sisal 78% (Brito et al., 2012).
can be seen in all spectra, regardless of the purification of the fibres.
However, it was lower than curaua 87% (Brito et al., 2012), bamboo
The intense peaks at 1656 cm−1 signified C]C cis stretching of un-
87% (Brito et al., 2012), eucalyptus 89% (Brito et al., 2012) and cotton
saturated acids or sterols correspond to tannin (Sun & Tomkinson,
linter 90% (Morais et al., 2013). Thus, the crystallinity value is de-
2002).
pending on different types of plants and the duration of fibres pur-
The intense peaks at 3200–3500 cm−1 indicated the present of OeH
ification and hydrolysis process. There are relation between the number
groups in untreated and treated fibres, due to presence of hydroxyl
of crystallinity degree region and the stiffness of cellulose, where in-
group in cellulose, hemicellulose and lignin. Peaks at 1800–1600 cm−1
crement in number of crystallinity region will raise the stiffness of fi-
signified carbonyl groups (C]O) in lignin and hemicelluloses
bres. Higher crystallinity in the chemical treated fibers is interrelated
(Kazayawoko, Balatinecz, & Woodhams, 1997). The high peaks at
with higher tensile strength of the fibers. Therefore, the mechanical
1000–1300 cm−1 was determined to be existing in all 4 types of fibres,
properties of the nanocomposite material can be improved by using
which signify CeH stretching and CeO groups, respectively (Faix et al.,
these treated fibers as nanofiller (Bhatnagar, 2005; Rong, Zhang, Liu,
1992).
Yang, & Zeng, 2001).

3.5. X-ray diffraction measurements

Various ordered crystalline arrangements were resulted from both
intra- and intermolecular hydrogen bonding occur in cellulose hydroxyl
groups. Fig. 4 shows the XRD patterns for sugar palm fibres at different
stages of treatment. The characterization of fibres polymoph can be
determined via diffractograms of XRD, in which it displayed a mixture
of polymorphs of cellulose I (typical peaks at 2θ = 15° and 22.6°) and
cellulose II (peaks at 12.3° and 22.1°) (Klemm et al., 2005). Fig. 4. also
shows the value of crystallinity index for sugar palm fibres, bleached
fibres, alkali-treated fibres and SPNCCs. Major intensity peak that was
identified in the X-ray diffractograms which located at 2θ value of
around 22.6° shown the crystalline structure of cellulose I for all sam-
ples, whereas the low intensity peak at a 2θ value of around 18° was
labelled as amorphous region (Segal et al., 1959).
The peak at around 2θ = 22.6° is sharper for chemically treated
3.6. Particle size measurement and zeta potential
Zeta potential (estimated as surface charge property of nanoma-
terial) and zeta sizer (particle size measurement) are analyzed using
Zetasizer Nano-ZS (Malvern Instruments, Worcestershire, UK). The
formation and the size of the SPNCCs obtained were also checked by
TEM. The result gained shows that the SPNCCs possessed a large ne-
gative charged, with mean value of −61.50 ± 1.65 mV. The strong
negative zeta potential value was measured, revealed the existence of
negatively-charged SPNCCs in the suspension. These large negatively-
charged zeta potential values were obtained due to the conversion of
the hydroxyl groups in to sulfate ester groups (e.g., conversion of cel-
lulose-OH to cellulose-OSO3−H + ), on SPNCCs surface during sul-
phuric acid hydrolysis treatment (Börjesson & Westman, 2015). The
suspension of NCCs were considered to be stable as the absolute value

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R.A. Ilyas et al. Carbohydrate Polymers 181 (2018) 1038–1051

Fig. 5. (i) TG and (ii) DTG curves for (a) raw sugar palm fibres, (b) bleached fibres, (c) alkali-treated fibres and (d) SPNCCs.

were larger than −27 mV (de Mesquita, Donnici, & Pereira, 2010). The
particle size distribution resulted in only one main group with 100% of
the particles were around 138.93 ± 13.93 nm. This light scattering
technique cannot measure the size of particle accurately and precisely
as it measured the length and diameter dimension of the particle
thoroughly. Nevertheless, the size distribution are ranging from
5.6–1106 nm are considered similar to the TEM measurement (Fig. 2).
According to Braun et al. (2008), these techniques could substitute TEM
for good estimation of NCCs dimensions, only if there is adoption of
adequate mathematical method. Thus, for SPNCCs, the Helmholtz–S-
moluchowski equation of general purposes was effective for measuring
the SPNCCs crystals’ dimensions.
3.7. Thermogravimetric analysis
It is crucial to study the thermal properties of the natural fibres in
order to determine their compatibility as nanofiller for biocomposite
processing, since the thermoplastic processing temperature would arise
above 200 °C. The thermogravimetric analysis data results obtained
from sugar palm fibers, as well as those obtained after bleaching, alkali
and hydrolysis treatment are shown in Fig. 5. Besides that, Fig. 5. also
illustrated both raw TG curves (panel i) and derived curves (DTG −
panel ii) as a function of temperature. Table 3 shows the comparison of
percentage weight loses for untreated and treated sugar palm fibres.
Generally, the thermal decomposition of raw sugar palm fibres was
divided into four phases. The initial phase was evaporation of moisture
content in fibres (occurred from 45 to ∼123 °C), next decomposition of
lignocellulosic components of hemicelluloses (occurred from 220 °C
to ∼315 °C), followed by cellulose (occurred from 315 to ∼400 °C),
lignin (occurred from 165 °C to ∼900 °C) and finally their ash
(1723 °C) as reported elsewhere (Ishak, Sapuan, Leman, Rahman, &
Anwar, 2012; Yang, Yan, Chen, Lee, & Zheng, 2007).
The initial weight loss started around 42 °C was caused by water
evaporation in these samples. As fibres are heated, there was reduction
in weight of the material initially. This was due to the loss of water and
volatile extractive, which they tend to move to the surface of fibres
(Rosa et al., 2010). The movement of volatile extractives happened due
to the migration of water from lower interior part of fibres to the higher
potential of water at the surface of fibres, as the water on the surface of
fibres was evaporated. Therefore, the migration of water was indirectly
carried the volatile extractive and left it on the fibres surface (Ishak
et al., 2012). It can be seen that the evaporation of moisture of (a) raw
sugar palm fibres was completely evaporated at 196.56 °C, compared to
the treated fibres (134–184 °C) as shown in Fig. 5. This is because of
higher moisture content (MC) of sugar palm fibres, resulted in higher
mass loss (10.38%) compared to the other treated fibres as shown in
Table 1. As the fibres were being treated, the weight loss were de-
creased due to lowered moisture content. Moreover, low mass losses
can be seen at low heating temperatures, which mainly linked with only
loss of water in cell lumen and in cell wall, and volatiles extractives in
the fibers, whereas huge mass losses that estimated up to 70% losses
were expected to be in form of basic constituent; starting from hemi-
cellulose, cellulose and lignin where they started to decompose at
temperature of 100 °C and above (Ishak et al., 2012; Yang et al., 2007).
The DTG curve of original sugar palm fibres displayed an earlier
weigh loss started at 210.58 °C, which then reached the highest peak at
281 °C, due to the low decomposition temperature of hemicellulose and
lignin (Morán et al., 2008). Hemicellulose was very easy to get rid of
from main steam and subsequently degrade into CO2, CO, and some
hydrocarbon, etc. at low temperatures between 220–315 °C. This is due
to the composition of hemicellulose which composed of various sac-
charides such as xylose, mannose, glucose, galactose, etc., and it’s
amorphous structure which appeared in random and rich of branches
(Yang et al., 2007). On the other hand, the cellulose fibers obtained by
bleaching treatment showed a higher decomposition temperature
around 345 °C, which was almost similar than those reported by Yang
et al. (355 °C) (Yang et al., 2007).
Table 3 shows the comparison of degradation temperature on
maximum weight-loss rate (TMax), weight loss (WL) and char yield for
treated and untreated sugar palm fibres obtained from the TG and DTG

Table 3
Onset temperature (TOnset), degradation temperature on maximum weight-loss rate (TMax), weight loss (WL) and char yield for raw sugar palm fibres, bleached fibres, alkali-treated fibres
and SPNCCs obtained from the TG and DTG curves.

Sample Water evaporation 1st thermal degradation 2nd thermal degrade Char yield

TOnset (°C) TMax (°C) WL (%) TOnset (°C) TMax (°C) WL (%) TOnset (°C) TMax (°C) WL (%) W (%)

Raw sugar palm fibres 41.73 106.78 10.38 210.58 281 15.13 308.05 345.45 43.76 30.73
Bleached fibres 42.37 103.74 9.87 195.66 271.56 15.24 288.35 324.44 52.39 22.5
Alkali-treated fibres 43.49 101.23 8.58 207.92 346.09 73.71 – – – 17.71
SPNCCs 43.72 103.43 7.37 185.78 348.65 78.41 – – – 17.97

1047
R.A. Ilyas et al.
curves. These outcomes clearly shows that the thermal stability of the
sugar palm fibres decreased after bleaching treatment and further in-
creased after alkali-treatment. The 1st degradation temperature was
found to be 281, 271.56 and 346.09 °C for the raw sugar palm fibres,
bleached-treated, and alkali-treated fibres, respectively. This is due to
the removal of the fiber structure, which facilitated degradation of the
remaining hemicellulose and lignin components from the fibres.
Bleaching treatment also led to fibres fibrillation, i.e. break down of the
fibres bundle into individual fibers (Deepa et al., 2011b). These process
enhanced the removal of fiber constituents like hemicelluloses, lignin,
and waxes from the fiber, resulting in elevated surface destruction with
well-defined fibril aggregates. The reduction in the value of tempera-
ture of bleached fibres compared to raw sugar palm fibres was expected
to occur due to the low lignin percentage in chemical composition of
bleached fibres as related in Table 1. In facts, lignin was the most dif-
ficult to decompose compared to cellulose and hemicellulose, which the
temperature of decomposition started early as 160 °C and extends as
high as 900 °C (Yang et al., 2007). Besides that, lignin also was a very
tough component and responsible for providing stiffness to the cell wall
as well as serving to bond individual cell together in the middle lamella
region (Ishak et al., 2012). As the lignin is removed via bleaching
treatment, the chemical component remaining in the fibers are mostly
composed of hemicellulose and cellulose. Thus, the degradation process
was easy to occur in alkali-treated fibers due to temperature degraded
of hemicelluloses are around 220–315 °C as hemicellulose has low
temperature degraded compared to other macromolecular components
i.e: cellulose and lignin (Shafizadeh & Chin, 1977).
Throughout the decomposition of the (a) raw sugar palm fibres and
(b) bleached fibres, a small peak appeared at 281 and 271.56 °C, re-
spectively, nearby to the main peak. This peak was attributed to the
decomposition of hemicellulose and lignin, then disappeared, as ex-
pected, in the case of the alkali-treated fibres (Fortunati et al., 2013).
Moreover, the weight loss is much more progressive than that of che-
mically purified samples. In addition, a shoulder is observed in the DTG
curve at around 300 °C, but is no longer present after the alkali treat-
ment, which likely reveals the removal of a partial of the hemicellulose
(Sheltami et al., 2012).
Moreover, (c) alkali-treated fibres illustrated an increase in the mass
loss temperature (WL = 73.71%; TMax = 346.09 for 1st degradation)
compared to raw sugar palm fibres (WL = 43.76%; TMax = 345.45 for
2nd degradation) and bleached fibres (WL = 52.39%; TMax = 324.44
for 12nd degradation). The degradation of cellulose in the fibres was
started within 315–400 °C (Yang et al., 2007). This proved the cap-
ability of the cellulose to sustain the heat deformation temperatures.
The alkali-treatment process helped to remove the lignin and hemi-
cellulose after bleaching treatment process as displayed in Table 1. The
mechanism of alkali-treatment involved the oxidation of hemicellulose
and lignin which led to dissolution of both component by breaking
down the polysaccharides to simple sugars and hence released the
cellulose fibers (Deepa et al., 2011b). The dissolution of these various
component via the bleaching and alkali process produced α-cellulose as
a residue material, which has been described to be crystalline
(Beckermann & Pickering, 2008). The higher the crystalline structure,
the higher the degradation temperature (Cherian et al., 2008). From
Table 3, we can see that there were increment in the degradation
temperature in (c) alkali- and (d) hydrolysis treated fibres (1st and 2nd
thermal degradation, respectively), due to the higher crystallinity
structure of fibres. This would indirectly enabled the fiber to endure
severe heat and processing conditions. The hydrolysis treatment was
proved to reduce long micro fibres chain to nano-dimention effectively,
by hydrolyzing the amorphous region. Thus, it can be summarized from
these results that the production of SPNCCs displayed an enhancement
of thermal properties of fibres than untreated fibres, which then making
them suitable as reinforcing materials in bio-renewable composite
material preparation.
The degradation temperature of sugar palm fibres after bleaching
1048
Carbohydrate Polymers 181 (2018) 1038–1051
and alkali treatments was around 200 °C, which was lower than that of
raw fibres. This result was similar as reported by Li et al. (2009) and
Soares et al. (1995) for mulberry barks cellulose and pure cellulose,
respectively. The degradation temperature become lower due to the
remained hemicellulose component after the chemical treatment in the
fibres. Hemicellulose was located between cellulose fibril. Thus, the
strong bonding between hemicellulose and cellulose fibril resulted to
decrease the crystallinity of cellulose fibrils and thus assessable the
beginning process of thermal degradation (Deepa et al., 2011b;
Petersson, Mathew, & Oksman, 2009).
This lower degradation temperature were caused by the hemi-
cellulose component, which remained after the chemical treatments.
Hemicellulose was located within and between the cellulose fibrils. This
strong association between hemicelluloses and cellulose fibrils was
believed to decrease the crystallinity of the cellulose fibrils and accel-
erate the beginning of the thermal degradation process.
The result shows that the fibers that undergo hydrolysis treatment
start to degrade earlier compared to other fibres, around
TOnset = 185.78 °C. This may be attributed to the residual of sulphuric
acid group within the fibre, thereby causing the degradation tempera-
ture of fibres to be lower. This lower degradation temperature
TOnset = 185.78 °C was also referring to the accessible degradation
temperature of highly sulfated amorphous region which acting as the
flame retardants (Roman & Winter, 2004b), whereas the higher tem-
perature phase correspond to the degradation of unsulfated crystal in-
terior. Though the fibres have been neutralized to pH of 6–7 during the
process of dilution, however there are still lagging of sulphuric acid
group present within the SPNCCs. It has been reported elsewhere
(Julien, Chornet, & Overend, 1993; Kim, Nishiyama, Wada, & Kuga,
2001; Li et al., 2009) that the thermostability of NCCs could be reduced
a lot due to the treatment of sulphuric acid hydrolysis, as this treatment
introduce sulfated group into the NCCs.
The oxidation and breakdown of the charred residue is occurred at
the final degradation phase (DTG peak above 425 °C), where these re-
sidues were converted to lower molecular weight gaseous products
(Flauzino Neto et al., 2013). Besides that, after the lignin had been
completely decomposed, the residue left was the inorganic material
which also assumed as ash content or char residue. This was due to the
presence of inorganic material such as silica (silicon dioxide, SiO2) in
the fibres which can only be decomposed at a high temperature over
1723 °C and above (Ishak et al., 2012). Moreover, less weight residue of
bleached fibres and alkali-treated fibres than that of raw sugar palm
fibres was because of the hemicellulose and lignin were removed from
the both bleached fibres and alkali-treated fibres, (Nguyen, Zavarin, &
Barrall, 1981), where this non-cellulosic could encourage high forma-
tion of char residue. Whereas for SPNCCs, the weight residue of SPNCCs
was increased due to the sulfate groups acting as the flame retardants
(Roman & Winter, 2004b). These results were very consistent with re-
sults obtained from the chemical composition, XRD and FTIR mea-
surements.
4. Conclusion
SPNCCs was successfully extracted and isolated from sugar palm
fibers using the treatment of delignification (NaClO2), mercerization
(NaOH) and hydrolysis (H2SO4). The chemical composition analysis
showed an increase trending in the cellulose content after each che-
mical treatment; it therefore changed from 43.88%% in the raw sugar
palm fiber to 81.5% in the bleached fibres and to 82.33% in the alkali-
treated fibres. FTIR results also showed that the chemical treatments of
delignification (NaClO2) and mercerization (NaOH) was effectively
used to remove lignin and hemicellulose, respectively.
Thermogravimetric analysis (TGA) shows that the thermal stability
increased in the materials having undergone chemical treatments. This
was due to the removal of hemicellulose and lignin as well as to an
increase in crystallinity during processing. XRD analyses pointed at a
R.A. Ilyas et al.
higher crystallinity for the chemically treated fibers, and the highest
crystallinity was found for the SPNCCs. Overall, the crystallinity in-
creased from 55.8% in raw sugar palm fibres to 65.9% in the bleached
fibres to 76.0% in the alkali-treated fibres and to 85.9% in SPNCCs.
TEM micrographs showed an adequate, random dispersion in solution
and revealed that sugar palm fibres can be recommended as a pre-
liminary material for the preparation of SPNCCs. The SPNCCs presented
a length (L) of around 130 ± 30 nm and average diameter (D)
9 ± 1.96 nm. This conducted experiment had revealed that sugar palm
fibres can be used as a starting material for the preparation of nano-
crystalline cellulose.
Acknowledgments
The authors would like to appreciate University Putra Malaysia for
financial support through the Graduate Research Fellowship (GRF)
scholarship. The authors are thankful to Dr. Muhammad Lamin
Sanyang for guideline throughout the experiment. The authors also
thanks the Forest Research Institute Malaysia (FRIM) and Dr. Rushdan
Ibrahim for their advice and fruitful discussions.
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