d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279

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Reinforcement of denture base resin with short

vegetable ber

Jie Xu a , Yan Li a, , Tao Yu a , Lei Cong b

a School of Aerospace Engineering and Applied Mechanics, Tongji University, Shanghai, China
b School of Dental Medicine, Tongji University, Shanghai, China

a r t i c l e i n f o a b s t r a c t

Article history: Objectives. Short ramie bers were selected to investigate the effect of ber length and volume
Received 31 March 2013 fraction on the exural properties of ramie ber reinforced denture base PMMA. With the
Received in revised form aid of measured interfacial shear strength and theoretical prediction values, experimental
19 July 2013 results were well interpreted.
Accepted 25 September 2013 Methods. Interfacial properties between denture base PMMA and ramie bers were evaluated
by single ber pull-out test. Then, chopped ramie bers were pre-stirred with PMMA powder
by a mechanical blender and then mixed with MMA liquid to fabricate composites. Two
Keywords: crucial inuencing factors, ber volume fraction and ber length, were studied to clarify
Denture base PMMA their effects on exural properties of composites.
Vegetable ber Results. With 1.5 mm bers addition, exural modulus of denture base PMMA rose from 2.50
Composite materials to 3.46 GPa with 10 vol.% bers, while exural strength declined steadily with increment of
Interfacial shear strength ber content. If ber length was 3.0 mm, the modulus showed a growth to 3.5 GPa at 4 vol.%
Flexural properties ber content followed by a drop to 3.00 GPa at 10 vol.%, whereas uctuation in strength
Dispersion was experienced. Experimental results were discussed by comparison with two theoretical
models.
Signicance. Short ramie ber reinforced denture base PMMA had higher exural modulus
than neat resin, while strength was lowered due to the weak interfacial adhesion. The poten-
tial of vegetable bers as reinforcing agents for denture base should be further investigated
by strengthening the interface between cellulose and denture base PMMA.
2013 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.

weight polyethylene ber (UHMWPE) [6,7], have attracted

1. Introduction
Reinforcing bers were introduced to the family of denture
base materials, in order to fulll their requirement on higher
mechanical properties against occlusal overload. Among the
wide varieties of used reinforcing agents, glass bers [15] and
several kinds of polymeric bers, e.g. ultra-high molecular
more attentions due to their high tensile properties and
acceptable esthetic appearance. However, when ber came
out from the surface of the resin as a result of degrada-
tion of resin or mechanical failure, clinical problems such as
mucosal irritation might happen [8,9]. Thus, not only rein-
forcing capacity but also clinical applicability of bers should
be considered during selections. As a result of this fact,

Corresponding author at: School of Aerospace Engineering and Applied Mechanics, Tongji University, 1239 Siping Road, Shanghai 200092,
China. Tel.: +86 021 65985919; fax: +86 021 65983950.
E-mail address: liyan@tongji.edu.cn (Y. Li).
0109-5641/$ see front matter 2013 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.dental.2013.09.013
1274 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279
Table 1 Chemical composition of ramie ber [16].
Component Percentage by mass
Cellulose 6799
Hemicellulose 1314
Pectin 1.92.1
Lignin 0.51.0
Fat/wax 0.3
investigations on the potential of alternative reinforcing
agents were ongoing.
In the range of naturally obtainable bers, vegetable ber
is one of the promising biomaterials due to its biocompat-
ibility [1013]. More importantly, they occupy much higher
Youngs modulus and ultimate tensile strength than denture
base resin. Therefore, these two inherent properties of veg-
etable bers make it worthwhile to characterize their potential
as new reinforcing agents for denture base. To authors best
knowledge, Kondo et al. [14] rst introduced short sisal ber to
denture base PMMA. Their results showed that with the incre-
ment of ber content, exural modulus of composites showed
a slight growth at 2.5 wt% and then a continuous decline up to
10 wt%, whereas exural strength decreased apparently and
uctuated versus ber content. On top of this, they suggested
that further studies should regard ber aspect ratio and sur-
face treatment.
Ramie is one of the oldest textile bers known as china
grass, which are referred as bast bers and come from the
phloem tissue of the plant [15]. It has signicantly smaller
diameter (1060 m) and consequently higher aspect ratio
than sisal ber (200300 m) at the same length. In addition,
its whiteness might also fulll the requirement of denture
base on esthetical appearance. Due to these facts, the present
work aimed to investigate the potential of ramie ber as a
reinforcing agent for denture base resin. In order to disperse
short ramie ber homogeneously in high-viscous denture
base PMMA, the approach of mechanical stirring was applied
during the fabricating stage. Specically, effects of ber vol-
ume content and length as well as dispersion and interfacial
property on exural properties of composites were detailedly
discussed.
2. Materials and methods
2.1. Materials
Heat-polymerizing denture base materials (Rapid Simplied )
were purchased from Vertex Dental, Netherlands and ramie
bers from Hunan province, China. Chemical composition,
physical and mechanical properties of ramie bers were listed
in Tables 1 and 2, respectively.
Long ramie bers were pre-impregnated in 5 wt% sodium
hydroxide solution, in order to remove wax and other impu-
rities from ramie ber [18], which was followed by washing
and then drying to drive out residual waters. 100 samples
of mercerized ramie bers were randomly selected and their
diameters were measured with the aid of an optical micro-
scope.
Table 2 Physical and mechanical properties of ramie
ber.
Property Valuea
Density (g/cm3 ) 1.50
Tensile strength (MPa) 310
Tensile modulus (GPa) 61.4128 [17]
Fractural elongation (%) 3.0
Tensile modulus was referred.
a
From laboratorial tests, averaged in normal distribution.
2.2. Fabrication of single ber pull-out specimens
In order to insure the single ber located centrally through-
thickness direction of the resin, two pieces of plastics with
rectangular grooves were cut off from the same plate. After-
wards plastic mold and ramie bers were positioned with
double-sided adhesive tape onto a stainless steel plate, then
mixed resin were injected into the overlapped groove with
a syringe. When the resin reached dough stage, plastic
mold was covered with another stainless steel plate and
then pressed under 1 MPa and heated at 100 degrees for
20 min, according to manufacturers instruction of curing
denture base PMMA. After demolding, specimens for single
ber pull-out test were chopped carefully from the groove
and 31 samples with matrix in regular shape were obtained
out of 40. Finally, diameters of bers and their embed-
ded lengths in the matrix were measured with an optical
microscope.
2.3. Fabrication of short ber reinforced composites
Mercerized ramie bers were carefully chopped with a scissor,
desiring to the length of 1.5 and 3.0 mm. 100 samples for both
lengths were randomly selected and measured with a vernier
caliper. The majority for the former proved to be 1.5 0.1 mm
and for the latter 3.0 0.2 mm.
Each group was divided into 4 sub-groups of different
weight. Then they were mixed with PMMA powder and stirred
with a blender at a rotating speed of 400 rpm (Fig. 1). After
5 min, bers randomly oriented in PMMA powder and MMA
was afterwards added to their mixture at a ratio of 0.6 ml/g
(liquid: powder). When the resin reached dough stage, it was
poured into a mold and hot-pressed under the same pressure
and temperature as in Section 2.2. After demolding, no visibly
seen bubbles existed in the composites by making the sam-
ples following the manufacturers (Vertex Dental) instruction.
Then, weight fractions of ber in composites were calculated
into volume fractions.
2.4. Mechanical testing
Single ber pull-out test was conducted at a crosshead speed
of 1 mm/min based on ASTM STP 452. According to ASTM
D7264, specimens for exural test were cut from molded com-
posites to the dimension of 64 mm 12.7 mm 3 mm and the
crosshead speed was also 1 mm/min.
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279 1275

Fig. 1 Schematic procedures of dispersion by mechanical stirring.

2.5. Calculation
3. Results
Apparent Interfacial Shear Strength IFSS was calculated from
3.1. Statistics of diameters of ramie bers
Eq. (1) [19]:
Scattering of ramie ber diameters was illustrated in Fig. 2.a.
Fmax
IFSS = (1) It was obvious that most diameters fell in the range from 25
 d le
to 45 m and the statistics normally distributed at 31.2 m,
where Fmax is the peak load, d the diameter of ber and le the which was one of the necessary parameters for later calcula-
embedded length of ber in the matrix. tion of theoretical exural modulus.
Critical ber length lc was then calculated from Eq. (2):
3.2. Interfacial shear strength and critical ber length
f
lc = d (2)
2IFSS Typical single ber pull-out process (Fig. 2.b) should include
(1) elastic deformation (intact interfacial bonding), (2) partial
where f is the ultimate tensile strength of ramie ber. debonding (crack was initiated at debond force Fd and propa-
Analytical exural modulus was expressed by Coxs model gated until complete debonding after peak force Fmax ) and (3)
(analytical) in Eq. (3): sliding friction [22]. In the test, 16 samples out of 31 underwent
the similar process and thus were considered valid data. After
Ecomp =  l Vf Ef + (1 Vf )Em (3) being calculated, interfacial shear stress averaged 2.35 MPa
with the standard deviation of 0.84, which implied an evi-
where  , l and Vf denote ber orientation factor, which is
dent scattering of the values. It was observed that the larger
0.375 for random-in-plane distribution [20], ber length factor
the diameters of ramie bers were, the more apparently IFSS
and volume fraction. Ef and Em are Youngs modulus of ber
dispersed. However, the effect of ramie ber diameter on the
and matrix, respectively. Specically, l was expressed by Eq.
interfacial shear strength should be further investigated.
(4):
Employing the strength of ramie ber (in Table 2), critical
ber length of 2.1 mm was obtained following Eq. (2).
tanh(L/2)
l = 1 (4)
L/2
3.3. Flexural properties of composites
and  could be deducted by Eq. (5):
Flexural modulus of composites versus ber volume fraction
 1/2 with ber length of 1.5 and 3.0 mm were compared in Fig. 2c.
2Em When ber length was 1.5 mm, exural modulus increased
= (5)
rf2 Ef (1 + m ) ln(1/Vf ) from 2.50 GPa of neat resin to 3.46 GPa of composites with
10 vol.% bers. When ber length was 3.0 mm, the modulus
Semi-empirical exural modulus was expressed by Halpin- showed a more dramatic growth and peaked at 3.5 GPa with
Tsais model (HT) in Eq. (6) [21]: 4 vol.% ber, which was followed by a drop to 3.00 GPa at the
maximal ber content.
3 5 3 1 + 2sL Vf Flexural strengths of composites were shown in Fig. 2d.
Ec = E11 + E22 = Em
8 8 8 1 L Vf With 1.5 mm bers, the strength declined gradually from
5 1 + 2sT Vf 90.5 MPa of neat resin to 78.7 MPa with 10 vol.% bers. By con-
+ Em (random-in-plane) (6)
8 1 T Vf trast, with 3.00 mm bers, strength of composites experienced
a deviant increment versus ber content.
where s denoted ber aspect ratio and L , T could be calcu-
lated from Eq. (7): 4. Discussion
Ef /Em 1 Ef /Em 1
L = , T = (7) Problems of unsatised dispersion of short ber in denture
Ef /Em + 2s Ef /Em + 2 base PMMA were widely discussed in previous studies [2327].
1276 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279

Fig. 2 (a) Scattering of ramie ber diameters; (b) a typical force-to-displacement-curve of single ber pull-out test; (c)
exural modulus and (d) exural strength of composites vs. ber volume fraction.

Initially, since the resin is high-viscous at the processing stage,
it has great difculty in permeating into the areas between
bers, which might introduce voids and porosity in compos-
ites and consequently reduces its strength in most cases.
Furthermore, the resin under pressure can shift the impreg-
nated bers apart due to even higher viscosity, which could
also cause inhomogeneous dispersion of bers in the matrix
[23,24]. These problems will be more apparent especially when
concentration of bers reaches a level of around 10% by mass
[25]. Therefore, it was concluded by many researchers that
in order to disperse short bers homogeneously, concentra-
tion of added bers should be limited within a low portion,
among which a critical content of 4% by mass was mostly
suggested [26,27]. Although low amount of bers agglomerate
hardly and voids in fabricated composites can be reduced to
an ideal level as a result of this, from micromechanical aspect
of short ber reinforcement, ber content contributes posi-
tively to their bearing capacity [19]. Therefore, increasing ber
content and achieving optimal dispersion need to be realized
at the same time.
In this study, experimental exural modulus was compared
with two kinds of theoretical models. All other parameters for
calculation were tested, as listed in Table 2. Due to laboratorial
limitation, Youngs modulus of ramie ber was referred to the
literature [17], where a range from 61.4 to 128 GPa was com-
monly used. When ber length was 1.5 mm, growth of exural
modulus had a similar trend with Coxs and Halpin-Tsais
models (Fig. 3a, overlapped experimental data were pointed by
arrows), despite the fact that gentle agglomeration at higher
contents slowed the rising rate (Fig. 4a). With ber in length of
3.0 mm, exural modulus also xed well with models at initial
stage (Fig. 3b), while it then fell steadily due to the fact that
bers in higher aspect ratio moved more difcultly and thus
agglomerated more easily (Fig. 4b).
Moreover, considering the theory of Maximum Packing
Fraction for randomly oriented short bers, expressed in Eq.
(9) [21]:
f
Vmax = kd/l (9)
the maximum ber volume contents, above which short bers
no longer have any rotational freedom, were 8% and 4% for
ber in length of 1.5 and 3.0 mm, respectively, which also agree
well with this study.
However, according to enhanced exural modulus at ini-
tial stage, it could be concluded that mechanical pre-stirring
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279 1277

5000 5000
length=1.5mm length=3.0mm
HT~Max HT~Max
4500 HT~Min 4500 HT~Min
Cox~Max Cox~Max
Cox~Min Cox~Min
Flexural modulus (MPa)

Flexural modulus (MPa)

4000 4000

3500 3500

3000 3000

2500 2500

0 0
0 2% 4% 6% 8% 10% 0 2% 4% 6% 8% 10%
a Volume fraction b Volume fraction

Fig. 3 Comparison of exural modulus and theoretical models: (a) ber length = 1.5 mm; (b) ber length = 3.0 mm.

Fig. 4 Status of dispersion of 10 vol.% short ramie ber in denture base PMMA: (a) ber length = 1.5 mm; (b) ber
length = 3.0 mm.

of PMMA powder with short ramie bers had a positive contri- factor l in Fig. 5. Apparently, with increment of ber length
bution to their dispersion, which did not introduce any other up to 1.5 mm, its factor increased exponentially to 0.8. After
material and operated easily within a few minutes. Effect of ber length exceeded 3.0 mm, it plateaued above 0.9, which
ber length on modulus was represented by its corresponding was usually considered as a sufcient value for modulus of

1.0 1.0

0.8 0.8
Fiber length factor
Fiber length factor

0.6 0.6

0.4 0.4
E=128
f
GPa E=61.4
f
GPa
Vf=0.103 Vf=0.103
Vf=0.066 Vf=0.066
0.2 0.2
Vf=0.037 Vf=0.037
Vf=0.012 Vf=0.012

0.0 0.0
0.0 1.5 3.0 4.5 0.0 1.5 3.0 4.5
Length of fibers (mm) Length of fibers (mm)
a b
Fig. 5 Fiber length factor l vs. increment of ber length: (a) Ef = 128 GPa; (b) Ef = 61.4 GPa.
1278 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) 12731279
Fig. 6 (a) Fractography of single ber pull-out specimen:
(a) schematic construction of outer layer and inner part of
ramie ber.
short ber composites. In other words, ramie ber in length of
3.0 mm should be a reasonable choice for denture base PMMA.
Other than exural modulus, exural strength is sensitive
to the interfacial adhesion. Single ber pull-out is one of the
most commonly used micromechanical tests for investigating
interfacial properties and further calculation of critical ber
length lc [19]. Although lc is an essential factor for design of
short ber reinforced composites, assumption of good interfa-
cial adhesion and uniform dispersion should not be neglected.
For the reason that the environment in which individual ber
located in a real composite varies from that in a single ber
pull-out specimen, especially at the content when interaction
between bers lowers the quality of wetting. Thus, exceed-
ing the critical ber length does not simply guarantee the
enhancement of ultimate strength, when dispersion becomes
an issue, which was also reected in this study. With 3.0 mm
bers, exceeding critical length of 2.1 mm, the composites had
lower strengths than expected values, which revealed that the
interface was not good. Supportingly, the weakness of inter-
face was conrmed by Fig. 6a, which pictured the peeling of
outer layer from ramie ber after single ber pull-out test. It
revealed the bonding between the outer layer and inner part of
ramie ber was deconstructed by the shear stress along their
interface I2 (Fig. 6b). So after I2 began to fail, the stress from
the matrix could not be sufciently transferred to the inner
part of ber. Thus, the ultimate strength of ramie ber was
not utilized to enhance the strength of composites.
The effect of ramie ber on PMMA is quantitatively com-
parable with that of glass ber, when both bers are short
and randomly distributed. For instance, as reported in [3],
exural modulus of PMMA was enhanced by 48%, and ex-
ural strength by 31% with 6 mm, 5% E-glass ber addition.
Therefore, by comparison with the reinforcing effects of ramie
bers, glass bers showed better effect on strength, but sim-
ilar effect on modulus. The difference of reinforcing effects
of ramie and glass ber mainly lay in their inherent prop-
erties. Glass ber occupies higher tensile strength, reaching
20003500 MPa [17], which is three to six times that of ramie
ber. Further research could be devoted to nd suitable sur-
face modication for ramie ber, to increase the efciency of
stress transfer in the composites. However, the biocompati-
bility and environmental friendly advantages of ramie bers
were much superior to glass bers. Therefore, there should be
some potential using of ramie bers in the dental applications.
Technically, ramie ber is usually offered in long form and
extra work is needed to cut it into the desired length. There-
fore, nding an efcient way to make short ramie bers is
important for the bulk production.
5. Conclusion
For 1.5 mm ramie bers reinforced denture base PMMA,
due to good dispersion, exural modulus of compos-
ites increased considerably with ber content approaching
10 vol.%. Although adding 3.0 mm bers increased the exural
modulus more rapidly up to 4 vol.%, they reduced the modulus
at higher contents as a result of apparent agglomeration. Flex-
ural strength of short ramie ber denture base PMMA declined
due to the weak interfacial adhesion.
From both experimental and theoretical studies, the criti-
cal ber length for ramie ber reinforced denture base PMMA
was 2.1 mm. With better interfacial bonding, higher exural
strength should be achieved.
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