Study on Depositing SiO2 Nanoparticles on the Surface of

Jute Fiber via Hydrothermal Method and its Reinforced

Polypropylene Composites

Haiyan Chen , Yihua Cui, Xuan Liu, Miao Zhang, Senjie Hao, Yuehong Yin
Institute of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing,
210000, China

To improve the interfacial compatibility of jute fiber reinforced composites less than expected, thus limiting their
reinforced polypropylene (PP) composites, hydrothermal applications.
method was used to deposit SiO2 nanoparticles on the
surface of pretreated jute fibers and the effect of reac- In the attempts to improve the interfacial compatibility
tion factors (tetraethoxysilane [TEOS] concentration, between natural fibers and polymer, many approaches including
ammonia concentration, and reaction temperature) on physical and chemical treatments have been conducted. Manalo
the deposition of SiO2 nanoparticles were evaluated. et al. [7] treated bamboo fibers with 6 wt% sodium hydroxide
The results of FTIR, XRD, SEM, and TEM showed that
solution, the tensile strength, bending strength, and stiffness of
the amorphous SiO2 nanoparticles with an average par-
ticle size of 65.0 nm were successfully deposited on the bamboo fiber reinforced polyester composites were increased
surface of jute fibers at the TEOS/H2O volume ratio of by 10%, 7%, and 25%, respectively. Girones et al. [8] treated
1:2, ammonia of 0.55 M, reaction temperature of 100
C sisal fibers with isocyanate, the tensile and bending strength of
(0.15 MPa) for 5 h. Compared with the sol–gel method, SiO2 sisal fiber reinforced polystyrene composites were enhanced by
nanoparticles obtained by the hydrothermal method pos-
sessed smaller particle size and were less agglomerated, 18% and 9%, respectively. However, the improvement in inter-
which can better fill in the surface defects of the jute fibers facial compatibility of natural fibers reinforced composites by
and result in a 12.9% increase in the tensile strength. The these treatments is limited.
study on the mechanical properties and interface perfor- Some studies [9] showed that introducing nanoparticles on
mance of the jute fiber reinforced PP composites indicated the surface of natural fibers could enlarge the interfacial area of
that the interfacial compatibility between jute fibers and PP
was obviously improved. The tensile and impact strength of the composites, which was beneficial to increase the efficiency
the composites reinforced with nano-SiO2 deposited jute of stress transfer and improve the interfacial compatibility
fibers were increased by 26.87% and 25.65%, respectively, between natural fibers and polymer. Shi et al. [10] introduced
compared with the untreated jute fibers. J. VINYL ADDIT. CaCO3 nanoparticles into kenaf bast fibers by inorganic nano-
TECHNOL., 2019. © 2019 Society of Plastics Engineers
particle impregnation technique, the tensile strength, and tensile
modulus of kenaf bast fiber reinforced PP composites were
INTRODUCTION
increased by 25.9% and 10.4%, respectively. Wang et al. [11]
In the recent years, the research and utilization of natural grafted TiO2 nanoparticles onto the surface of flax fibers, and
fibers as a reinforcing material have gradually attracted the interfacial shear strength between flax fibers and epoxy
attention, and their compounding with thermoplastic poly- resins was enhanced by 40.5%. Liu et al. [12] found that SiO2
mer is a hot research topic in the field of polymer composite nanoparticles were deposited on the surface of jute fibers
materials. Natural fibers as a composite reinforcement possess via sol–gel method, and the tensile strength of the jute fiber was
many advantages over synthetic fibers, such as biodegradabil- enhanced by 17.9%, and the thermal property of jute fiber was
ity, light weight, low cost, high specific strength, and specific improved. Moreover, nanoparticles attached to the surface of
modulus [1–4]. At present, natural fibers reinforced composite natural fibers can increase the surface roughness of the natural
materials have been widely used in automobile, construction, fibers and produce strong mechanical interlocking between nat-
transportation, and aerospace industries [5]. However, the ural fibers and the polymer, thereby enhancing the interfacial
interfacial compatibility between natural fibers and non-polar bonding strength of the composites [13]. Therefore, introducing
polymer is poor due to the abundant hydroxyl groups in the nanoparticles on the surface of jute fibers is an effective method
cellulose [6]. This makes the performance of the natural fibers to improve the interfacial compatibility of the composites.
In this article, hydrothermal method was employed to
deposit SiO2 nanoparticles on the surface of the jute fibers.
Correspondence to: Y. Cui, e-mail: cuiyh@[Link] The effects of TEOS concentration, ammonia concentration,
DOI 10.1002/vnl.21714
Published online in Wiley Online Library ([Link]).
and reaction temperature on the micro-morphology of nano-
© 2019 Society of Plastics Engineers SiO2 deposited jute fiber were investigated, and the growth

Journal of Vinyl and Additive Technology—2019

mechanism of SiO2 nanoparticles on the surface of the jute the above solution under ultrasonic irradiation (300 W and
fibers was also discussed in this article. Subsequently, the com- 25
C). The time of ultrasonic irradiation was 1 h. Subse-
posites were fabricated using the nano-SiO2 deposited jute quently, the mixture was transferred into a Teflon-lined
fibers as the reinforcement and PP as the matrix, the mechanical stainless-steel autoclave and kept at 100
C for 5 h. Finally, the
properties and fracture surface of which were characterized to hydrothermal product was washed with ethanol for 3 times
evaluate the interfacial compatibility of the composites. and dried at 60
C for 3 h. In this reaction system, four TEOS
concentrations (0.01, 0.03, 0.05, and 0.07 M), four ammonia
EXPERIMENTAL concentrations (0.45, 0.55, 0.65, and 0.75 M) and four reaction
temperatures (80
C, 0.12 MPa; 90
C, 0.13 MPa; 100
C,
Materials 0.15 MPa; 110
C, 0.19 MPa) were tested (Table 1). The vol-
ume ratio of distilled water to TEOS was 2:1.
Tetraethoxysilane (TEOS), anhydrous ethyl alcohol, and
ammonia were provided by Sinopharm Chemical Reagent
Characterization of the Jute Fiber Deposited with SiO2
Co., Ltd (China). Sodium hydroxide and sulfuric acid (98%)
Nanoparticles
were purchased from Nanjing Chemical Reagent Share Co.,
Ltd (China). Jute fibers with an average diameter of 18 μm Morphology Analysis. The surface morphology of jute
were provided by Qingdao Derong Textile Co., Ltd (China), fiber before and after treatment was observed by a scanning
and cut to a length of 50 mm. Polypropylene(PP) films electron microscopy (SEM, S-4800, Hitachi Ltd., Japan).
(150 mm × 120 mm × 0.1 mm) were obtained from Nanjing Prior to the observation, all jute fiber samples were sputter
Julong Science & Technology Co., Ltd (China). coated with gold to enhance the conductivity.

Pretreatment of Jute Fibers The Deposition Amount of SiO2 Nanoparticles. The

deposition amount can reflect the deposition of SiO2
The surface of the jute fibers was covered by the low- nanoparticles on the surface of jute fiber to some extent.
strength colloid, which was easy to peel off from the jute The pretreated jute fibers were dried at 60
C for 3 h and
fiber trunk [5]. Hence, the acid/alkali pretreatment was weighed in an electronic balance (0.0001 g precision).
adopted to remove the surface colloid of the jute fibers. After depositing SiO2 nanoparticles on the surface of jute
Jute fibers were treated with 4 g/L sulfuric acid solution fiber, the nano-SiO2 deposited fibers were also dried at
for 30 min in the ultrasonic bath (300 W and 25
C). Then, 60
C for 3 h and weighed in an electronic balance. The
the treated jute fibers were washed to neutral with distilled deposition amount of SiO2 nanoparticles was finally calcu-
water and immersed in 8 wt% sodium hydroxide solution at lated by the following equation.
98
C for 1 h. After the treatment, jute fibers were washed
thoroughly with distilled water in order to remove the residual m2 − m1
m ð %Þ = × 100 ð1Þ
sodium hydroxide and dried at 60
C for 3 h. m1

where m is the deposition amount of SiO2 nanoparticles,

Deposition of SiO2 Nanoparticles m1 is the weight of the pretreated jute fibers before the
Depositing SiO2 nanoparticles on the surface of pretreated deposition, m2 is the weight of nano-SiO2 deposited fibers
jute fibers was carried out by hydrothermal method. A total of after the deposition.
0.1 g of the acid/alkali-treated jute fibers were placed into the
solution composed of 30 mL ethanol and a certain amount of X-Ray Powder Diffraction (XRD). The crystal phase of
TEOS, and then ethanol (10 mL)/distilled water solution and jute fiber before and after treatment was revealed by X-ray
ethanol (5 mL)/ammonia solution were sequentially added to powder diffraction (XRD, Miniflex-600, Bruker Co., Ger-
many) with Cu Kα radiation (λ = 1.5406 Å), and the 2 θ
ranges from 5
to 60
.
TABLE 1. Hydrothermal deposition conditions.
Fourier Transform Infrared (FTIR) Spectroscopy.
Temperature V(H2O)/
(
C) Time (h) TEOS (M) Ammonia (M) V(TEOS) The surface chemical groups of jute fibers before and after treat-
ment were analyzed by a FTIR spectrometer (Nicolet Nexus
100 0.01 0.55 870, Nicolet Co.), from wavenumbers of 4,000 cm−1 to
100 0.03 0.55 400 cm−1.
100 0.05 0.55
100 0.07 0.55
100 5 0.05 0.45 2:1 Transmission Electron Microscope (TEM) Analysis.
100 0.05 0.65 Jute fibers before and after deposition were fixed into a cap-
100 0.05 0.75 sule of epoxy resins and then cut into slices with a thickness
80 0.05 0.55 of about 50 nm perpendicular to the fiber axis. The jute fiber
90 0.05 0.55
slices were observed by the transmission electron micro-
110 0.05 0.55
scope (JEM-1011, Japan Electronics Co., Ltd., Japan).

2 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl

Tensile Tests of Single Jute Fiber. The tensile strength Ltd, China), according to ASTM D638 and ASTM D256,
of single jute fiber before and after treatment was tested in respectively.
a computer-controlled tensile tester (YG001A, Hongda
Co., Ltd., China) at a loading speed of 0.00125 mm/s at Mechanical Properties Testing. The tensile strength of
room temperature, according to ASTM D3379. The gauge the jute fiber reinforced PP composites was tested with
length of the individual jute fiber was 30 mm. At least Instron 3,369 (load cell 5 kN). The loading speed during
40 single jute fibers were tested for each surface treatment. the tensile testing was 2.5 mm/min, and five specimens
were tested for each jute fiber treatment.
The impact strength of the jute fiber reinforced PP com-
posites was performed on a XJU-5.5 Charpy impact tester.
Preparation and Characterization of the Jute Fiber The impact result was the average value for ten specimens.
Reinforced PP Composites
Preparation of the Jute Fiber Reinforced PP Composites. Interface Performance Analysis. The fracture surface of
Jute fibers before and after treatment were dispersed in the the composites obtained from the tensile tests was observed by
distilled water by continuous and vigorous mechanical stir- scanning electron microscope (S-4800, Hitachi Ltd., Japan) to
ring, and then jute fiber suspension was quickly poured into evaluate the interface performance, and all the specimens were
a 150 mm × 120 mm deckle box in a sand core funnel con- gold coated prior to observation.
nected to a vacuum pump. Finally dried in an oven at 105
C
for 12 h, jute fiber mats with a thickness of 1.36 mm were RESULTS AND DISCUSSION
formed.
Composites containing about 35% jute fibers by weight Effect of Hydrothermal Process Parameters on the
were fabricated by compression molding using the film- Morphology of SiO2 Nanoparticles
stacking method, as shown schematically in Fig. 1. Twelve
The SEM images of jute fiber before and after pre-
layers of jute fiber mat and thirteen layers of PP film were
treatment were shown in Fig. 2. It can be seen that the
alternately laid, and then the whole laminate was placed
untreated jute fiber consisted of bundles of fibrils and pres-
between two steel platens of a flat vulcanizing machine
ented quite smooth surface owing to the covering of the
(Y/TD7145A, Tianjin Tianforging Press Co., Ltd., China)
colloid (Fig. 2a and b). After the acid/alkali pretreatment,
at 180
C. The pressure was controlled at 1.5, 3.5, and
the surface of the jute fibers became rougher, and a number
5.0 MPa for 3 min, respectively, and then 15.0 MPa for
of parallel grooves of different sizes were distributed along
20 min. The plates of jute fiber reinforced PP composites
the longitudinal direction of the jute fiber (Fig. 2c and d).
with a thickness of 2.03 mm were obtained.
The results of SEM observation demonstrated that the col-
The plates were cut into standard specimens for tensile
loid had been removed from the surface of jute fibers.
and impact properties testing using a universal sampler
(XWAY-2, Xiamen Chongda Intelligent Technology Co.,
TEOS Concentration. Figure 3 showed the effect of TEOS
concentration on the deposition amount and the size of SiO2
nanoparticles on the surface of jute fibers. It can be seen that the
deposition amount of SiO2 nanoparticles on the surface of jute
fibers increased gradually with the increase of TEOS concentra-
tion. What is more, SiO2 nanoparticles were mainly distributed
in the grooves of the jute fiber surface (Fig. 4). Because
the grooves were more favorable for the nucleation of SiO2
nanoparticles than the convex portion of the jute fiber [14].
When the TEOS concentration was 0.05 M, uniform SiO2
nanoparticles could completely fill in the surface flaws of jute
fibers (Fig. 4c). Compared to the grafted TiO2 nanoparticles on
the surface of flax fibers reported by Wang et al [11], SiO2
nanoparticles deposited by hydrothermal method had less
visible agglomeration. As the TEOS concentration exceeded
0.05 M, SiO2 nanoparticles were easy to aggregate owing to the
limited nucleation sites on the jute fiber surface [12]. Therefore,
0.05 M could be considered to be the optimum TEOS concen-
tration for depositing SiO2 nanoparticles on the surface of jute
fibers via hydrothermal method.

Ammonia Concentration. As can be seen in Fig. 5,

ammonia concentration had a significant influence on the
FIG. 1. Fabrication procedure of jute fiber reinforced PP composites. deposition amount and the size of SiO2 nanoparticles on

DOI 10.1002/vnl Journal of Vinyl and Additive Technology—2019 3

 FIG. 2. SEM images of (a,b) untreated jute fiber, (c,d) acid/alkali-treated jute fiber.

the surface of the jute fiber. Ammonia, as the catalyst, deposited in the grooves of the jute fiber surface at an
could accelerate the hydrolysis of TEOS and condensation ammonia concentration of 0.55 M (Fig. 6b). This phenom-
reaction [15]. When the ammonia concentration was lower enon had never been reported and studied in the previous
than 0.55 M, the hydrolysis rate of TEOS was slower, researches on the modification of natural fibers with
which made it difficult for the hydrolyzed product to nucle- nanoparticles by a sol–gel method. High temperature and
ate through effective collision, so few SiO2 nanoparticles high pressure were the unique advantages of the hydrother-
were observed on the surface of the jute fiber (Fig. 6a). mal method, the synergistic effect of which promoted the
Dense and orderly arranged SiO2 nanoparticles were orientation arrangement of nanoparticles. This helped to
effectively fill in the surface defects of the jute fibers,
thereby improving the interfacial compatibility of the compos-
ites. When ammonia concentration exceeded 0.65 M, the
coagulation of SiO2 nanoparticles was observed (Fig. 6d). It
was attributed to the fact that high concentration of ammonia
induced the condensation reaction between the residual reac-
tive groups of SiO2 nanoparticles. Therefore, 0.55 M ammo-
nia could be considered to be the optimum ammonia
concentration for depositing SiO2 nanoparticles on the surface
of jute fibers via hydrothermal method.

Reaction Temperature. Figure 7 showed the effect of

reaction temperature on the deposition amount, and the size
of SiO2 nanoparticles on the surface of jute fibers. It can be
seen that as the reaction temperature rose, the deposition
amount of SiO2 nanoparticles on the surface of jute fibers
FIG. 3. The deposition amount and average size of SiO2 nanoparticles was gradually increased. This was because the increased
on the surface of jute fibers with different TEOS concentrations. the reaction temperature could promote the hydrolysis of

4 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl

 FIG. 4. SEM images of SiO2 nanoparticles deposited on the surface of jute fibers at different TEOS concentrations.

TEOS and condensation reaction, resulting in the increased with an average particle size of 29.0 nm, which possessed
deposition amount. high specific surface energy and made it easy to aggregate.
Nevertheless, the average size of SiO2 nanoparticles Therefore, 100
C was considered to be optimal reaction
deposited on the surface of jute fibers became smaller with temperature for depositing SiO2 nanoparticles on the sur-
a rising reaction temperature. When the reaction tempera- face of jute fibers via hydrothermal method.
ture was 80
C, the average size of SiO2 nanoparticles was  
92.0 nm. As the reaction temperature was 100
C, the aver- J = Aexp −
W
ð2Þ
age size of the SiO2 nanoparticles was reduced to 65.0 nm. kB T
According to the relationship between nucleation rate and
reaction temperature [16], as shown in Eq. (1), the nucle- where J is nucleation rate, A is a kinetic pre-exponential
ation rate was increased exponentially with the increase of factor, which is believed to be weakly dependent on tem-
reaction temperature, consequently SiO2 nanoparticles with perature T, kB is the Boltzmann’s constant, and W is the
smaller particle size were generated under the same hydro- reversible work of formation of critical nucleus.
thermal reaction conditions of TEOS concentraton, ammo- Furthermore, the average size of SiO2 nanoparticles depos-
nia concentration, and time. When the reaction temperature ited by hydrothermal method was much smaller than that of
was 110
C, aggregation occurred (Fig. 8d). This was SiO2 nanoparticles obtained by sol–gel method [12,17], thus
because explosive nucleation produced SiO2 nanoparticles grooves on the surface of the jute fibers could be better filled

FIG. 5. The deposition amount and average size of SiO2 nanoparticles FIG. 7. The deposition amount and average size of SiO2 nanoparticles
on the surface of jute fibers with different ammonia concentrations. on the surface of jute fibers at different reaction temperatures.

FIG. 6. SEM images of SiO2 nanoparticles deposited on the surface of jute fibers at different ammonia concentrations.

DOI 10.1002/vnl Journal of Vinyl and Additive Technology—2019 5

 FIG. 8. SEM images of SiO2 nanoparticles deposited on the surface of jute fibers at different reaction temperatures.

in, which avoided the formation of interfacial voids in the com- covering the surface of jute fiber, as shown in Fig. 4. With
posites. In addition, the smaller the size of SiO2 nanoparticles, the prolongation of reaction time, plenty of the fully hydro-
the higher the specific surface area. This could enlarge the inter- lyzed species, Si(OH)4, were produced, which are three-
phase area of the composites and enhance the interfacial bond- dimensionally open and fractal in structure and have four
ing between jute fibers and PP [9]. Therefore, hydrothermal equal functional groups (Si OH). They can act as the pri-
method might be an effective method for modifying jute fibers mary nuclei or the core of the particles to induce the forma-
with nanoparticles. tion of spherical SiO2 nanoparticles.
The formation of SiO2 nanoparticle nucleus was divided
into homogeneous nucleation and heterogeneous nucle-
Mechanism of Formation of SiO2 Nanoparticles on the
ation. The nucleus was directly formed from the hydrolysis
Surface of Jute Fibers. Based on the results mentioned
products of TEOS without the aid of foreign media, called
above, the mechanism of the formation of SiO2 nanoparticles
homogeneous nucleation. On the contrary, the nucleus was
on the surface of jute fibers was proposed and shown in Fig. 9.
formed by the hydrolysate of TEOS depending on the
The whole reaction system was mainly based on the
external medium (such as jute fiber), called heterogeneous
hydrolysis of TEOS precursor and subsequent condensa-
nucleation. In the hydrothermal deposition system, jute
tion of the resultant hydroxyl groups with the aid of basic
fibers acted as an effective substrate to promote the nucle-
catalyst. The detailed chemical reactions were shown in
ation and growth of SiO2 nanoparticles. Because based on
Eq.(3–8).
the homogeneous nucleation and heterogeneous nucleation
Hydrolysis
[17], as shown in Eq. (9–12), the free energy of heteroge-
neous nucleation was lower than that of homogeneous
SiðOC2 H5 Þ4 + H2 O ! ðOC2 H5 Þ3 SiðOHÞ + C2 H5 OH ð3Þ
nucleation, which means that SiO2 nanoparticles tend to
ðOC2 H5 Þ3 SiðOHÞ + H2 O ! ðOC2 H5 Þ2 SiðOHÞ2 + C2 H5 OH preferentially grow on the surface of jute fibers.
ð4Þ
4
ðOC2 H5 Þ2 SiðOHÞ+ 2 + H2 O ! ðOC2 H5 ÞSiðOHÞ3 + C2 H5 OH ΔG1 = − πr3 K B T ln ðSÞ + 4πr2 γ ð9Þ
V
ð5Þ 2Vγ
r* = ð10Þ
ðOC2 H5 ÞSiðOHÞ3 + H2 O ! SiðOHÞ4 + C2 H5 OH ð6Þ 3K B T ln ðSÞ
1

Condensation ΔG2 = 2 − 3 cos θ + cos 3 θ × ΔG1 ð11Þ
4
1

2X3 SiOH ! X3 Si-O-SiX3 + H2 O ð7Þ f ðθÞ = 2 − 3 cos θ + cos 3 θ ð12Þ
4
X3 SiOH + ðOC2 H5 ÞSiX3 ! X3 Si-O-SiX3 + C2 H5 OH ð8Þ
where ΔG (ΔG1 for the homogeneous nucleation and
ðX = -O-CH2 -CH3 ;-OHÞ
ΔG2 for the heterogeneous nucleation) is the sum of the
free energy of a new volume formation and a few surface
It can be seen that the hydrolysis of TEOS is a step-by-
created, V is the molecular volume of the precipitated spe-
step process, thereby producing four kinds of hydrolyzed
cies, r is the radius of the nucleus, r* is the critical radius
species: (OC2H5)3Si(OH), (OC2H5)2Si(OH)2, (OC2H5)Si
of the nucleus, KB is the Boltzmann constant, S is the sat-
(OH)3, Si(OH)4, and the order of the hydrolysis velocity is
uration ratio, γ is the surface free energy per unit surface
Eq (6)<Eq (5)<Eq (4)<Eq (3) [15]. Herein, in the initial
area, f(θ) is the surface factor, θ is the contact angle
stage of the reaction, the mainly existed hydrolyzed prod-
between the nucleus and substrate.
ucts might be (OC2H5)3Si(OH), (OC2H5)2Si(OH)2, and
(OC2H5)Si(OH)3, which are not three-dimensionally open
in structure. Subsequently, a portion of these hydrolyzed
Characterization and Properties of Jute Fibers
species could be adsorbed onto the jute fiber surface
through strong hydrogen bonds and electronic interactions FTIR Analysis. The characteristic spectra of the jute fibers
and were cross-linked with each other to form a thin film with different surface treatments were displayed in Fig. 10.

6 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl

 (a) C2H5 C2H5
O O OH OH OH
4C2H5 O Si O C2H5+ 10H2O hydrolysis C2H5 O Si OH + C2H5 O Si O C2H5 + HO Si OH + HO Si OH + 10C2H5OH

O O OH O OH
C2H 5 C2H5 C2H5

(b)

FIG. 9. (a) Hydrolysis of the TEOS, (b) schematic illustration of the deposition of SiO2 nanoparticles on the jute fiber surface.

The band at 3410 cm-1 was attributed to the stretching vibra- Fiber-OH + HO-SiO2 ! Fiber-O-SiO2 + H2 O ð13Þ
tion of hydroxyl groups [18]. The peak at 1740 cm-1 was
related to C O stretching vibration of COOH in hemicel-
lulose and pectin [19]. The peak at 1000 cm−1 was attrib- TEM Analysis. Figure 11 showed the TEM photographs
uted to the vibration of C O C [11]. The peak at of cross sections the acid/alkali-treated jute fiber and nano-
895 cm−1 corresponded to the vibration of anhydro-D- SiO2 deposited jute fiber (0.05 M TEOS, 0.55 M ammonia,
glucose [5]. For the acid/alkali-treated jute fiber, the charac- 100
C, 5 h), respectively. After hydrothermal deposition,
teristic band at 1740 cm−1 entirely disappeared, suggesting SiO2 nanoparticles were uniformly distributed on the sur-
that the colloid had been thoroughly removed from the jute face of the jute fiber to form a particle layer possessing a
fiber surface [12,19]. After depositing SiO2 nanoparticles via thickness of about 65.0 nm. Moreover, SiO2 nanoparticles
hydrothermal method, the peaks (451 cm−1 and 804 cm−1) were tightly bound to the jute fibers without gaps, which fur-
related to Si O Si appeared, which further proved that ther revealed that chemical bonding was formed between jute
nanoparticles deposited on the surface of jute fibers were fibers and SiO2 nanoparticles.
SiO2 [12,20]. The presence of Si O C peak at 1064 cm−1
indicated the formation of chemical bond between jute fibers XRD Spectra Analysis. The XRD pattern of jute fibers
and SiO2 nanoparticles. The intensity of peak at 3410 cm−1 with different surface treatments was shown in Fig. 12.
was weakened, and this was due to the condensation reac- The diffraction peaks at 15
, 16.7
, 22.8
, and 34.5
were
tion of hydroxyl groups between jute fibers and SiO2 indexed to the lattice planes at 101, 101, 002, and
nanoparticles, resulting in the reduction of free hydroxyl 040, respectively, which were characteristic peaks of the
groups on the surface of jute fibers (Equation 13). This cellulose fibers [21,22]. After the acid/alkali treatment, the
result showed the agreement with previous researches [14]. intensity of the diffraction peaks was enhanced. This was
Furthermore, the condensation reaction of hydroxyl because the acid/alkali treatment removed amorphous col-
groups between jute fibers and SiO2 nanoparticles was loid from the surface of jute fibers, which increased the
endothermic, and higher temperature in the hydrothermal proportion of cellulose and thereby resulted in increased crys-
process could promote the reaction compared to the sol– tallinity. As for nano-SiO2 deposited jute fiber, the intensity
gel method, which may facilitate the formation of stron- of the peak at 22.8
was much lower than that of the
ger and more C O Si bonds between SiO2 and jute acid/alkali jute fiber, and no new characteristic peaks
fibers. appeared. These results demonstrated that SiO2 nanoparticles

DOI 10.1002/vnl Journal of Vinyl and Additive Technology—2019 7

FIG. 10. FTIR spectra of the untreated jute fiber, acid/alkali-treated jute fiber, and nano-SiO2 deposited jute fiber. [Color figure can be viewed at
[Link]]

deposited by hydrothermal method were amorphous and decrease in the tensile strength of the jute fibers. Compared
overlapped with the peaks of cellulose at 22.8
[23]. Like- with the acid/alkali-treated jute fiber, the tensile strength
wise, the decrease in the intensity of the peaks at 15
and and modulus of nano-SiO2 deposited jute fiber was
16.7
was assigned to the amorphous SiO2 nanoparticles cov- enhanced by 19.5% and 12.3%, respectively, indicating
ering the surface of jute fibers. that the deposition of SiO2 nanoparticles could significantly
improve the tensile properties of the jute fibers. The result
Tensile Strength. The tensile strength of the jute fibers could be ascribed to two aspects: (1) SiO2 nanoparticles
with different surface treatments was given in Table 2. The increased the density of the jute fibers and reduced surface
untreated jute fiber had a tensile strength of 450 MPa. After flaws by filling in the grooves and micropores, thus
the acid/alkali pretreatment, the tensile strength and tensile diminishing the stress concentration on the jute fiber sur-
modulus of jute fibers was decreased by 5.6% and 4.2%, face during the tensile tests [10]; (2) the formation of
respectively. The removal of the colloid on the surface of Si O C between jute fibers and SiO2 nanoparticles also
the jute fibers exposed lots of grooves, which were consid- made it easier for stress transfer, yielding the improvement
ered as stress concentration areas, thereby resulting in a in the tensile strength of jute fibers [11].

FIG. 11. TEM images of jute fibers cross section: (a) acid/alkali-treated jute fiber, (b) nano-SiO2 deposited jute fiber.

8 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl

FIG. 12. XRD pattern of the untreated jute fiber, acid/alkali-treated jute fiber, and nano-SiO2 deposited jute fiber. [Color figure can be viewed at
[Link]]

The tensile stress–strain curve of the jute fibers with dif- was shown in Fig. 14. Compared with PP, the tensile
ferent surface treatments was shown in Fig. 13. It can be strength of the untreated jute fiber/PP composites was in-
seen that the linear region followed the initial nonlinear creased by 26.63%, indicating that jute fiber was an excellent
portion. The nonlinear behavior appeared to be the result composite reinforcement. Compared with the untreated jute
of jute fibers twisting [19]. Cellulose consisted of crystal- fiber/PP composites, the tensile strength of the acid/alkali-
line region and amorphous region. The cellulose macromo- treated jute fiber/PP composites and nano-SiO2 deposited jute
lecular chains in the amorphous region were disorderly fiber/PP composites were enhanced by 17.76% and 26.87%,
arranged along the jute fiber axis [11]. When the single jute respectively. After the acid/alkali treatment, the exposed
fiber was continuously stretched, macromolecular chain grooves increased the surface roughness of the jute fibers. This
would be oriented along the jute fiber axis until the jute was expected to provide a strong mechanical interlock between
fiber broke. As a result, the jute fibers exhibited the linear jute fibers and PP [26]. As for the nano-SiO2 deposited jute
behavior. It was widely acknowledged that the surface fiber/PP composites, SiO2 nanoparticles filling in the surface
flaws of the natural fibers had a negative impact on the ten- flaws of the jute fibers could avoid the formation of voids at
sile strength [24]. Hence, nano-SiO2 deposited jute fiber the interface of the composites and thus enhance the interfacial
exhibited the highest elongation at break. bonding between jute fibers and PP. Furthermore, SiO2
Based on the above experimental results, we studied the nanoparticles with high specific surface area would increase
effects of nanoparticle modification methods on the properties the interfacial area of the composites, which allowed the stress
of the natural fibers, and the results were shown in Table 3. to be transferred from PP to jute fibers more efficiently [9].

Impact Strength. Figure 15 showed the impact strength of

Performance of Jute Fiber Reinforced PP Composites jute fiber-reinforced PP composites with different surface
Tensile Properties. The tensile strength of jute fiber treatments. Compared with PP, the impact strength of the
reinforced PP composites with different surface treatments untreated jute fiber/PP composites was decreased by 27.22%.
This may be explained by the fact that the addition of jute
TABLE 2. Tensile properties of jute fibers with different surface treatments. fibers disrupted the continuity of the PP matrix. Moreover,
jute fibers may generate stress concentrations, which could
Tensile Tensile initiate microcracks in the matrix, and result in the reduced
Samples strength (MPa) modulus (GPa) impact performance of the composites [27]. Compared with
the untreated jute fiber/PP composites, the impact strength of
Untreated jute fiber 450  40.2 21.2  1.9
Acid/alkali-treated jute fiber 425  38.4 20.3  1.4 the acid/alkali-treated jute fiber/PP composites and nano-SiO2
Nano-SiO2 deposited jute fiber 508  32.9 22.8  1.2 deposited jute fiber/PP composites were increased by 7.48%.
and 25.65%, respectively. The increase in impact strength

DOI 10.1002/vnl Journal of Vinyl and Additive Technology—2019 9

FIG. 13. Tensile stress–strain curve of the untreated jute fiber, acid/alkali-treated jute fiber, and nano-SiO2 deposited jute fiber. [Color figure can be
viewed at [Link]]

TABLE 3. Effectiveness of depositing SiO2 nanoparticles on the surface of jute fibers via hydrothermal method.

Nanoparticles Natural fibers

Reference number Pretreatment Modification method Diameter (nm) Aggregation Degree of repair Tensile strength (%)

[25] - sol–gel 131.0~271.0 aggregation lower -

[12] acid/alkali treatment sol–gel 83.3 less aggregation low 17.9
this paper acid/alkali treatment hydrothermal 65.0 - higher 19.5

might be an outcome of the improved interfacial compatibility acted as a protective layer to prevent the cracks propagation
between jute fibers and PP. In the case of the nano-SiO2 and increase the energy dispersion. In addition, the interaction
deposited jute fiber/PP composites, SiO2 nanoparticles pos- between SiO2 nanoparticles and the components of the com-
sessed a toughening effect. When the composites were sub- posites, including the C O Si chemical bonding and the
jected to external force, SiO2 nanoparticles at the interface strong mechanical locking, resulted in the formation of a

FIG. 14. Tensile strength of jute fiber-reinforced PP composites with dif- FIG. 15. Impact strength of jute fiber reinforced PP composites with dif-
ferent surface treatments: (a) PP; (b) untreatment; (c) acid/alkali treatment; ferent surface treatments: (a) PP; (b) untreatment; (c) acid/alkali treatment;
(d) nano-SiO2 deposition treatment. (d) nano-SiO2 deposition treatment.

10 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl

FIG. 16. Fracture surface of jute fiber reinforced PP composites with different surface treatments: (a) untreatment; (b) acid/alkali treatment; (c) nano-SiO2
deposition treatment.

strong interface between jute fibers and PP, the damage of jute fiber were amorphous. The results of FTIR and TEM indi-
which would consume extra energy. These behaviors can cated that SiO2 nanoparticles were tightly bonded to the jute
enhance the impact strength of the composites. fibers through C O Si chemical bonds. Compared with
untreated jute fibers, the tensile strength of the nano-SiO2
deposited fiber was increased by 12.9%. SiO2 nanoparticles
Interface Performance Analysis. The fracture surface of
and the C O Si bonds generated between jute fibers and
the composites obtained from the tensile tests was analyzed
SiO2 nanoparticles were responsible for the improved perfor-
through SEM to evaluate the interfacial bonding strength mance of the jute fibers.
between jute fibers and PP. As shown in Fig. 16a, the 3. The mechanical property and fracture surface of the composites
untreated jute fibers were pulled out, and visible gaps can were studied. The results showed that depositing SiO2 nanoparticles
be seen between jute fibers and PP. This implied that the on the surface of the jute fibers via hydrothermal method could
interfacial bonding between untreated jute fibers and PP was remarkably improve the interfacial compatibility of the composites.
weak. For the acid/alkali-treated jute fiber/PP composites, the Compared to untreated jute fibers, the tensile and impact strength of
gap between jute fibers and PP became smaller, as shown in nano-SiO2 deposited jute fiber/PP composites were enhanced by
Fig. 16b. In case of nano-SiO2 deposited jute fiber/PP com- 26.87% and 25.65%, respectively. Microscopic investigation of the
posites, simultaneous failure of jute fibers and PP was fractured surfaces of the composites revealed enhanced interfacial
bonding between PP and jute fibers.
observed, and jute fibers were tightly bonded to the PP with-
out gaps (Fig. 16c). It was also noted that much PP adhered
to the surface of the jute fibers, indicating strong interfacial
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12 Journal of Vinyl and Additive Technology—2019 DOI 10.1002/vnl