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MAGAZINE OF CHEMISTRY T. 53(3) 379-384 JUNE 2015

DOI: 10.15625/0866-7144.2015-00148

MECHANICAL PROPERTIES OF COMPOZIT MATERIALS USING

PREPREG ON THE BASIS OF REINFORCED PHENOLIC AND EPOXY
PLASTIC FIBER FIBER AND GLASS-ARAMIT
Nguyen Huy Tungfirst*, Tran Vinh Dieufirst, Dang Huu Trungfirst, Doan Thi Yen Oanh1.2

firstResearch Center for Polymer Materials, Hanoi University of Science and Technology

2 Natural Science and Technology Publishing House, Vietnam Academy of Science and Technology
To the Editorial Office 11-4-2015; Accepted to post June 20, 2015

Abstract
Prepreg composite materials are becoming increasingly common in their industry due to ease of use, consistent properties
and high surface quality. However, there is much to understand about prepreg prior to committing to using this material.
Therefore, in this paper phenolic resin (rezolic) and two compositions, including solid epoxy resin DER633U/ Hardener DEH84
and epoxy Epikote 828/Hardener Novolac have been evaluated for preparing glass fiber and glass- aramid fibers reinforced
prepregs. Results showed that all single resin and compositions mentioned above are satisfied technical requirements for
prepregs. The best prepreg was made by composition DER633U/DEH84 because it possesses good shelf life at temperature 36-
37oC and high composite mechanical properties. For example, tensile strength 205.2 MPa and Izod impact strength 228.9 KJ/m2
with C-glass fabric reinforcement 360 g/m2.
Keywords. Prepreg, composite materials, epoxy resin, phenolic resin.

1. INTRODUCTION Because the technology of using prepreg is not yet

widely available in our country and there are a number of
chemical and technical problems to be solved, this work
Prepreg is a form of semi-finished product made from
focuses on studying some combinations of resin substrates
fabric, mat in flat form impregnated with resin, preserved
and prepreg preservation time. and evaluate the
for future use by wet laying method (manual pressing) or
mechanical properties of composites made from prepreg
other forming methods [1- 4]. In the prepreg, the fibers are
based on phenol-formaldehyde resin and glass fiber
aligned in the 0 . directiono and pre-impregnated with resin
reinforced hot curing epoxy.
is called co-directional strip. Some prepregs are available
in the form of co- directional strips, woven fabrics, or
2. US EXPERIMENT
continuous swaddle yarns. The co-directional strip gives
the ability to change the properties of the composite
2.1. Materials and chemicals
according to the design intent. Textile prepreg is used to
fabricate intricately shaped parts, where flexibility of the
Self-synthesized rezolic resin from phenol,
material is key. In general, prepreg can be classified into
formalin 37 % with ammonia catalyst 25 %, take 5 %
thermoset-based prepreg and thermoplastic-based prepreg.
compared with phenol. All are Chinese technical
Reinforcing fibers can be glass, carbon and aramid.
chemicals used directly without refining. Synthetic
Due to the prepreg preparation at the factory, the
rezolic resin has the following technical characteristics:
prepreg method has a number of advantages
Melting temperature 80-84oC; density 1.4802 g/cm3;
compared to the direct manual pressing method as
content of hydroxyl group 21.06%; free phenol content
follows: 1) Precise control of the fiber/resin ratio; 2)
2.16%; free formaldehyde content 9.37 %.
Achieve a higher fiber content; 3) Precise control of Novolac resin is self-synthesized from phenol and
product thickness and 4) Minimization of toxic for formalin 37% with 37% HCl catalyst, taking 1% compared
workers due to volatile chemicals and solvents. with phenol. Synthetic novolac resin has the following
technical characteristics: 109 . softening temperatureoC;
density 1.2623 g/cm3; content of hydroxyl group 15.8

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TCHH, Ward 53(3), 2015 Nguyen Huy Tung and associates

%; free phenol content 3.9%; free formaldehyde
content 0.86%.
- Epikote 828 epoxy resin (Shell Chemicals) has
epoxy group content 22.63%.
- Solid epoxy resin DER663U (Dow Plastics) has
epoxy group content 4.79%.
- DEH84 (Dow Plastics) curing agent has
hydroxyl equivalent 240-270 g/eq, is the reaction
product of liquid epoxy resin with bisphenol A,
containing 1.9% promoter.
- Crystalline tertiary amine catalyst DMP-30 (Merck)
pure.
- 360 g/m . C-glass cloth2 and 450 g/m2
(China).
- E-glass fabric 610 g/m2 (USA).
- Glass cloth MB4500 silane treatment 550 g/m2
(Australia).
- Aramid fabric 200g/m2 (Australia).
mass of the sample after extraction compared to the mass of the
original sample.
2.2.3. Method to determine the mechanical properties of
polymer composite materials
Tensile strength was determined on a machine
INSTRON 5582-100 KN (USA) according to ASTM
D638, tensile speed 2 mm/min.
Bending strength was determined on a machine
INSTRON 5582-100 KN (USA) according to ASTM D790,
bending speed 2 mm/min.
Charpy impact strength was determined on a
Radmana ITR-2000 machine (Australia) according to ISO
179-1993. Test speed 3.5 m/s.
Izod impact strength was determined on a Tinius
Olsen machine (USA), according to ISO 180:1993 (E).
The specimen is notched in a V shape with a notch
angle of 45±1 .0. Test speed 3.5 m/s.

2.2. Analytical methods and techniques used 3. RESULTS AND DISCUSSION

2.2.1. Chemical analysis 3.1. Research on manufacturing composite materials
based on glass fiber reinforced rezolic resin
Epoxy group content: The epoxy group content was
determined by the method of mercury nitrate with 3.1.1. Effect of temperature and time on gel
HCl/dioxane reaction solution [5]. content
Hydroxyl group content: Determination of the hydroxyl group
content by esterification of the hydroxyl group with acetic
The curing process of rezolic resin has been investigated at the
anhydride in the presence of piridin [6].
temperature of 140, 150 and 170 . oC over time. The obtained results
Free phenol content: Determination of free are shown in figure 1.
phenol content by bromination according to
Koppeschaar method [6, p.16].
Free formaldehyde content: Determination of
free formaldehyde content by sulfite method [7].

2.2.2. physicochemical analysis

FTIR infrared spectra were determined on a

Perkin Elmer GX 600 (USA).
DTA and TGA thermal analysis were performed on
a Shimadzu thermal analyzer (Japan) in nitrogen
atmosphere, the heating rate was 10 oC/min from 25 to
500 oC with a platinum crucible.
Determination of Brookfield Viscosity: Viscosity Figure 1: herEffect of temperature and arrival time
was determined according to DIN 53018 on a
gel fraction of rezolic resin.
Brookfield Model RVT-Series 93412 viscometer
(USA) at 25 oC.
From Figure 1, it can be seen that, in order to match the
Determination of gel fraction (curing degree): The
hot pressing condition in the mold, the condition of curing
gel fraction was determined by extraction method in
rezolic resin at 150 oC for 30 minutes. Under these
Soxhlet kit with acetone. The gel fraction is the part that
conditions, the gel fraction reached 94 %.
forms the spatial network that is not extracted by
acetone in the Soxhlet set with a time of 15-16 hours.
The gel fraction content is the ratio 3.1.2. Mechanical properties of composite materials based
on glass fiber reinforced rezolic resin and aramite

Used ethanol solvent to dissolve the resin

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TCHH, Ward 53(3), 2015 Mechanical properties of composite materials…

rezolic. To facilitate the process of impregnating the resin solution

onto the glass cloth (prepreg preparation) a concentration of 40%
was chosen for the ethanol resin rezolic. The viscosity of the
rezolic resin solution was almost unchanged during the 30 days of
investigation at room temperature (Figure 2).
Types of fiberglass reinforcement include: C-glass 450
g/m2, E-glass 610 g/m2 and hybridized E-glass 610 g/m2 with
aramite 200 g/m2. The obtained results are presented in Table
1. From Table 1, it can be seen that the obtained composite
materials have good mechanical properties. In the case of
hybrid E-glass fabric 610 g/m2
and aramid fabric 200 g/m2 according to the intercalation method, the tensile
strength reached 230.2 MPa.

Figure 2: The time-viscosity dependence of rezolic resins

in ethanol solvents at room temperature

Table 1: Mechanical properties of composites based on rezolic resins

Content Mass Tensile Bending strength Impact resistance

Reinforced yarn
yarns (%) separately (g/cm3) (MPa) (MPa) (KJ/m2)
C-glass 450 g/m2 62.2 1.613 116.2 127.6 46.3
E-glass 610 g/m2 65.8 1,744 198.7 178.9 60.3
E-glass 610 g/m2
/aramite 200 g/m2 57.6 1.423 230.2 216.0 49.2

Processing mode of composite materials from prepreg: Heating at 80 oC/1 hour, raise the
temperature to 150 oC and maintained for 30 min. Pressing pressure 50-60 KG/cm2.

3.2. Research on manufacturing composite materials based

on epoxy resin Epikote 828/Novolac reinforced with glass
fiber

3.2.1. Investigate the effect of DMP-30 catalyst on

gel content of Epikote 828/Novolac . combination

Novolac resin is used here as a curing agent

for epoxy resins. To accelerate the curing process,
a DMP-30 catalyst was used. Effect of catalyst
content DMP-30 on the degree of curing of
Epikote 828/Novolac complex at 120oC is shown in
figure 3.
From Figure 3, it can be seen that the suitable
conditions for curing Epikote 828/Novolac Time, minutes
combination: Temperature 120
Figure 3: herEffect of catalyst content DMP-30
oC for 30 min, with 0.5% DMP-30 catalyst. Under
these conditions, the gel content reached 95%. to the degree of curing of the Epikote . complex
828/Novolac at 120 oOLD
3.2.2. Mechanical properties of glass fiber
reinforced Epikote 828/Novolac composites Mechanical properties of composites obtained from
prepreg are presented in Table 2.
From Table 2, it can be seen that the mechanical properties
Used acetone/solvent mixturen-butanol = 1/1 volume to
of composite materials on the basis of Epikote 828/ Novolac with
dissolve Epikote 828/Novolac combination at 45%
the same fiber reinforced C-glass 450 g/m2
concentration for easy penetration into glass cloth to form
prepreg. The viscosity of Epikote 828/Novolac solution All have higher values than composite materials using
gradually increased after 10 days (Figure 4). rezolic resin (Table 1), especially impact strength is 32 %
higher (up from 46.3 KJ/m2).2 up 61.3 KJ/m2).

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 TCHH, Ward 53(3), 2015 Nguyen Huy Tung and associates

3.3. Research on manufacturing composite materials

based on glass fiber reinforced epoxy resin DER663U/
DEH84

3.3.1. Effect of DEH84 curing agent on gel

content of DER663U/DEH84 combination

The DEH84 curing agent content changed by the

value of 30, 32, 34, 36 and 38 PKL compared with 100
PKL of epoxy resin DER663U. The curing process is
carried out at a temperature of 190 .oC. The effect of
DEH84 curing agent on the gel content of the assembly
is shown in Figure 5.
Figure 4: The dependence of the viscosity on
time of
Epikote 828/Novolac in solvent mixture
exeton/n-butanol at room temperature

Table 2: Mechanical properties of composite materials on the basis of

Epikote 828/Novolac/DMP-30 fiberglass reinforced

Reinforced yarn
Content Mass Tensile Bending strength Impact resistance
yarns(%) separately (g/cm3) (MPa) (MPa) (KJ/m2)
C-glass 450g/m2 57.0 1.627 144.3 156.6 61.3
Note: Step-by-step heating, at first at 90 oC/1 hour, then raised to 1200/30 minutes. Pressing pressure 50-60 KG/cm2.

Figure 5: The dependence of the gel fraction on

DEH84 content at 190 oOLD Figure 6: herEffect of curing time on
curing degree of DER663U/DEH84 . combination

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TCHH, Ward 53(3), 2015
From Figure 5, it can be seen that, when increasing the
concentration of DEH94 curing agent from 30 to 38 PKL, the gel
content increases from 92% to 98%, corresponding to the curing
agent content of 30 PKL and 38 PKL.
3.3.2. Effect of time on the degree of curing of the
DER663U/DEH84 combination at 190 oOLD
The curing agent content of DEH84 varies from 30
PKL to 38 PKL compared to 100 PKL of epoxy resin
DER663U. The curing reaction is carried out at
190 .oC. The results of the survey on the change in gel
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Nguyen Huy Tung and associates
From Figure 6, it can be seen that, in all surveyed
samples, the curing reaction occurs quickly after 2
minutes. At that time, the gel content of the samples
reached about 20%. Samples with higher curing agent,
gel content was also higher, but not significantly. The
curing reaction occurs fairly rapidly over a period of 2 to
4 minutes. After 4 minutes, the gel content has reached
98%. Next, the gel content increased very slowly. This
curing mode allows quick fabrication of composite
samples from prepreg.
The results of infrared spectroscopy show that, in epoxy
sample DER663U, there are peaks of 1290 cm-first and 827 cm-first
TCHH, Ward 53(3), 2015 Mechanical properties of composite materials…

characterize the valence vibration of epoxy group and

peak 3427 cm-first specific for the hydroxyl group. After
curing, pic 3432 cm-first has a much stronger absorption
strength. Meanwhile pic 826 cm-first and 1253 cm-first typical
for epoxy group, the absorption strength decreases very
quickly.

3.3.3. Thermal analysis survey results TGA and DTA

The results of DTA thermal analysis of the DER663U/

DEH84 combination are presented in Figure 7.

Figure 8: TGA diagram of the combination

DER663U/DEH84

From Figure 8 it can be seen that the DER663U / DEH84

combination has very high thermal stability. At temperatures
below 400oC the mass loss is negligible. Above 400oC the loss
increases with temperature and has a very strong decrease in
mass at 441 oC. Approaching 500 oC the material is almost
completely decomposed, the mass loss at this temperature is
90%.

3.3.4. Effect of the number of layers of reinforced glass fabric on

Figure 7: DTA diagram of the DER663U/DEH84 . combination
From Figure 7 it can be seen that the curing reaction of
epoxy resin DER663U with DEH84 occurs strongly at 151oC.
The results of TGA thermal analysis of the DER663U/
DEH84 combination are presented in Figure 8.
the mechanical properties of composite materials
Fabricated two types of material samples with different number
of layers of glass fabric with different weights per square meter with
the background of the DER663U/DEH84 combination. Samples are
made in a mold with a pressure of 50 KG/cm2, at a temperature of
190 oC for 6 min. The obtained results are presented in Table 3.

Table 3: herEffect of the number of layers of reinforced glass fabric on the mechanical properties of composite materials
Drag Curling Durability and
Content
TT Combination
yarns (%) Reliability Modules Reliability Modules dam
(MPa) (GPa) (MPa) (GPa) (KJ/m2)
DER663U/DEH84
first
/crystal cloth 78.5 205.2 2.7 115.3 8.1 228.9
C-360 g/m2, 17 classes
DER663U/DEH84
2 /crystal cloth 76.2 164.6 2.4 97.0 9.0 186.5
C-450 g/m2, 13 layers

From Table 3, it can be seen that the number of layers of
reinforcing fabric greatly affects the mechanical properties of
composite materials. When increasing the number of fabric layers
from 13 layers to 17 layers, all mechanical properties increase.
Tensile strength increased from 164.6 MPa to 205.2 MPa (increased
24.6%), tensile modulus increased covariably with tensile strength
from 2.4 to 2.7 GPa; flexural strength increased from 97.0 MPa to
115.3 MPa (up 18.8%) but the flexural modulus decreased from 9.0
to 8.1 GPa. This is true because the function
As the amount of glass fiber increases, the tensile strength increases and
the flexural strength decreases as the amount of resin decreases. Notched
Izod Impact Strength increased from 186.5 KJ/m2 up 228.9 KJ/ m2 (up
22.7%).
3.3.5. Prepreg shelf life
The shelf life or shelf life of prepreg is very
important because it determines the shelf life

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TCHH, Ward 53(3), 2015
storage, storage and transportation of products.
Surveyed the lifetime of prepreg made from
DER663U/DEH84/glass fabric, over time
Table 4: Curing degree of prepreg made from combination DER663U/DEH84/type C glass fabric
Life time 1 week 2 weeks
Gel fraction (%) 0 0
From Table 4, it can be seen that the shelf life of
prepreg is quite good, stored at high temperature above
36-37 . oC in the summer like this, but after 4 weeks, the
gel content was only 9.8%. Increasing the storage time to
5, 6, and 7 weeks, the gel content increased slowly and
reached 15.6 % after 7 weeks. So this type of prepreg if
stored at room temperature 25oC or lower, the lifetime will
be longer.
4. CONCLUSION
Effectively used rezolic resin and two other
combinations, epoxy resin Epikote 828/Novolac and
epoxy resin DER663U/DEH84 as the substrate for glass
fiber reinforced prepreg.
The viscosity of rezolic solution in ethanol did not change
after 30 days at room temperature, indicating that rezolic resin
is suitable for prepreg preparation.
Viscosity of Epikote 828/Novolac solution in
acetone/solvent mixturen-butanol gradually increased
after 10 days at room temperature (25-30 oC).
Therefore, it is necessary to store prepreg at a
temperature below 10 .oC to prolong life.
Direct survey of prepreg based on epoxy resin
DER663U/DEH84 found at quite high temperature 36- 37
oC in the summer, but after 7 weeks the gel content only
increased to 15.6 %. Thus, the DER663U/DEH84
combination is very suitable for prepreg fabrication.
The mechanical properties of the composites made from the
prepregs of this work are good and depend on the type of reinforced
glass fiber or hybrid with aramid fiber. But the most prominent is the
composite material made from prepreg based on the
DER663U/DEH84 combination, the tensile strength reached the
highest value of 205.2 MPa when only increasing
Contact: Nguyen Huy Tung
Research Center for Polymer Materials Hanoi
University of Science and Technology No. 1,
Dai Co Viet, Hai Ba Trung, Hanoi E-mail:
tungnh@gmail.com.
384
Nguyen Huy Tung and associates
(weeks), stored at temperatures above 36-37 oC (summer in
Hanoi). The obtained results are presented in Table 4.
3 weeks 4 weeks 5 weeks 6 weeks 7 weeks
0 9.8 12.7 13.5 15.6
reinforced with glass cloth 360 g/m2 and impact
strength also reached the highest value 228.9 KJ/m2
with this reinforced glass fabric.
Thank you. The work was completed with the
financial support of the State Project, code DT-
PTNTĐ.2012-G/01. The authors thank the Laboratory
of Polymer and Composite Materials, Hanoi
University of Science and Technology, for creating
favorable conditions during the implementation.
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