Dental Materials Journal 2011; 30(6): 954–959

Preparation and characterization of thermoplastic materials for invisible

orthodontics
Ning ZHANG1, Yuxing BAI1, Xuejia DING2 and Yu ZHANG2

Department of Orthodontics, School of Stomatology, Capital Medical University, Beijing, 100050, China
1

Key Laboratory of Beijing City on Preparation and Processing of Novel Polymer Materials, Beijing University of Chemical Technology, Beijing, China
2

Corresponding author,  Yuxing BAI;  E-mail:  byuxing@263.net


PETG/PC/TPU polymer blend was prepared by mechanical blending. The mechanical properties of modified PETG/PC/TPU blend
were characterized using a universal testing machine, and results were compared against two commercial thermoplastic products
—Erkodur and Biolon. Blending modification improved the properties of PETG/PC/TPU. When blending ratio (wt%) was 70/10/20,
PETG/PC/TPU exhibited optimal mechanical properties which exceeded those of Erkodur and Biolon. Tear strength was 50.23 MPa
and elongation at break was 155.99%. Stress relaxation rate was 0.0136 N/s after 1 hour, which was significantly slower than
Erkodur and Biolon (p<0.05). Water absorption rate was 0.57% after 2 weeks, which was significantly lower than Erkodur and Biolon
(p<0.05).

Keywords: Invisible orthodontics, Thermoplastic materials, Blend, Modification



stability9). Despite the plethora of thermoplastic

INTRODUCTION
Thermoplastic materials have been widely used for
orthodontic retainers, temporomandibular joint splints,
night guards, and bleaching trays1,2). This wide range of
applications stems from several key inherent advantages
of thermoplastic materials: simple to use, excellent
esthetic characteristics, and superior formability.
Recently, the use of thermoplastics in orthodontic
treatment is further fuelled by the use of CAD/CAM
technology in the design and fabrication of thermoplastic
appliances3,4).
Clear thermoplastic appliances are well received as
they are more esthetically appealing than traditional,
stainless steel, fixed appliances. However, orthodontists
reported that 70% to 80% of their patients required
midcourse correction, case refinement, or conversion to
fixed appliances before the end of treatment5,6). Efficacy
of tooth movement with clear thermoplastic appliances
was also lower than with fixed appliances7). These
lackluster clinical results clearly showed that the
application of thermoplastic materials for orthodontic
tooth movement requires a sufficient understanding of
the material characteristics, optimal material selection,
and design.
Unlike traditional orthodontic techniques, the
quality of orthodontic force exerted by a clear
thermoplastic appliance depends on the mechanical
properties of the fabrication material8). In other words,
to achieve the desired treatment outcome through
orthodontic interventions, a thorough study for a critical
understanding of the mechanical properties of the
different thermoplastic materials is essential and
mandatory.
For an orthodontic material, the desirable properties
are large springback, low stiffness, good formability,
high stored energy, biocompatibility, and environmental
products available in the market, none of which is
designed for orthodontic tooth movement when measured
against this list of critical characteristics. Therefore, to
improve the efficacy of tooth movement with invisible
orthodontic appliances, it is important to develop a new
thermoplastic material which possesses this
comprehensive list of desirable properties.
Currently, polyester, polyurethane, and
polypropylene are the predominant thermoplastic
materials used to fabricate clear orthodontic appliances.
Poly(ethylene terephthalate)-glycol (PETG), a non-
crystallizing amorphous copolymer of polyethylene
terephthalate (PET), has good mechanical properties,
formability, optical qualities, fatigue resistance, and
dimensional stability. For these excellent properties,
PET and PETG play an important role within the rapidly
growing family of thermoplastic elastomers (TPE) and
their applications can be found in almost all industrial
branches10-12). Polycarbonate (PC) is a very durable
material and can be laminated to make bullet-proof
glass. It has characteristics that resemble those of
polymethyl methacrylate (PMMA), but PC is stronger
and usable in a larger temperature range. This
thermoplastic material is also highly transparent to
visible light and has better light transmission
characteristics than many kinds of glass13-15).
Thermoplastic polyurethane (TPU) is one of the
most versatile engineering thermoplastics with
elastomeric properties. It combines the mechanical
properties of vulcanized rubber with the processability of
thermoplastic polymers. It can be repeatedly melted and
processed due to the absence of chemical networks that
normally exist in rubber. TPU possesses a myriad of
favorable properties: excellent physical properties,
chemical resistance, abrasion resistance, adhesion
characteristics, and ease of processing. Therefore, TPU’s

Received May 16, 2011: Accepted Aug 30, 2011

doi:10.4012/dmj.2011-120 JOI JST.JSTAGE/dmj/2011-120
 Dent Mater J 2011; 30(6): 954–959
applications run the gamut from engineering materials
and coatings to adhesives and films16,17).
Polymer blending has been accepted as an efficient
and inexpensive method of polymer property
diversification18,19). To obtain a useful product with a
satisfactory level of cohesion, various structural
considerations of the blend partners should be considered
so as to obtain a blend that may be classified as miscible
or mechanically compatible20). To date, a considerable
amount of literature on polyester blends has been
published: PETG/PET, PETG/LCP, PC/ABS, PC/PP,
TPU/PVDF, TPU/PP, and TPU/PMMA10,17,21-25). These
studies showed that polymer blending was indeed an
effective way to improve the mechanical properties of
polymers, eventually culminating in a high-performance
engineering material.
The objective of this study was to improve the
mechanical properties of PETG/PC/TPU polymer blend
by blending modification to meet the list of critical
characteristics required of invisible orthodontic
appliances. The mechanical properties of the prepared
PETG/PC/TPU polymer blend were characterized and
then compared against those of two commercial
thermoplastic products, Erkodur and Biolon.
MATERIALS AND METHODS
Raw materials for polymer blending
Three polymers were selected as raw materials to
prepare the polymer blends in this study: poly(ethylene
terephthalate)-glycol with a molecular weight of 26,000
(PETG; DN011, Eastman Chemical Co., Tennessee,
USA), polycarbonate with a molecular weight of 23,500
(PC; P5001, Unitika, Osaka, Japan), and thermoplastic
polyurethane with a molecular weight of 18,000 (TPU;
345X, Bayer, Leverkusen, Germany). They were
supplied in the form of translucent, colorless pellets.
Three types of polymer blends were prepared in this
study: PETG/PC, PETG/TPU, and PETG/PC/TPU. For
each type of polymer blend, five different blending ratios
(wt%) were used. For PETG/PC, the five blending ratios
of PETG to PC were: 100/0, 90/10, 80/20, 60/40, and 40/60
(w/w). For PETG/TPU, the five blending ratios of PETG
to TPU were: 100/0, 95/5, 90/10, 85/15, and 80/20 (w/w).
For PETG/PC/TPU, the five blending ratios in respective
orders were: 80/10/10, 70/10/20, 60/10/30, 50/10/40, and
40/10/50.
Polymer blend specimens were obtained by injection
molding process in accordance with ISO standard 527-2
type 1A. Before injection molding, the pellets were dried
in an oven for 6 h at a temperature of 80°C. Table 1
summarizes the injection molding conditions used in this
study.
Table 1 Injection molding conditions of polymer blends
Tube machine
Mold temperature Injection time
temperature
240 °C 80 °C
955
Erkodur (1.0 mm thickness; Erkodent Erich Kopp
GmbH, Pfalzgrafenweiler, Germany) and Biolon (1.0 mm
thickness; Dreve Dentamid GmbH, Unna, Germany) are
two widely used commercial thermoplastic products.
They were used in this study for benchmarking
comparison of the mechanical properties of the prepared
polymer blend materials.
Tear strength measurement
Rectangular specimens, 5 mm×40 mm, of each polymer
blend material were prepared for tear strength testing.
The tear strengths of all rectangular test specimens were
measured according to ASTM guideline D624-00, which
measures the force required to completely rupture across
the width of a material26). Tear strength testing was
carried out using a universal testing machine (Model
3300, Instron, Norwood, MA, USA) at room temperature
and at a crosshead speed of 10 mm/min. For each
polymer blend material, the mean value of five test
specimens was calculated.
Stress relaxation measurement
Rectangular specimens, 5 mm×40 mm, of each polymer
blend material were prepared for stress relaxation
testing. Dimensions of the test specimens before and
after stress relaxation testing were taken according to
ASTM guideline D624-00. Using a universal testing
machine, all test specimens were loaded at room
temperature to reach a 5% strain. They were then
unloaded and allowed to recover for 60 minutes (i.e.,
3600 seconds). Stress relaxation rate was calculated as
follows: (N0–N1)/3600, where N1 is the residual stress of
specimen after 60 mins and N0 is the initial stress before
stress relaxation testing. For each polymer blend
material, the mean value of five test specimens was
calculated.
Water absorption measurement
Rectangular specimens, 50 mm×50 mm, of each polymer
blend material were prepared for water absorption test.
Specimens were stored in a desiccator to reach a constant
weight (W0) before they were immersed in distilled water
at 37°C. To measure weight gain ratio, specimens were
periodically retrieved from the water at 6, 12, 24, 48,
168, and 336 h after immersion began. At each retrieval,
specimen was wrapped in filter paper to absorb water
from the surface and then weighed using an electronic
balance. Reading accuracy was 0.1 mg and variation in
specimen weight was less than 0.12%.
Percent increase in weight (%) was calculated as
follows: [(Wt−W0)/W0]×100, where Wt is the specimen
weight at immersion time t and W0 is the initial specimen
weight before immersion. Percentage of water absorbed
Injection pressure Cooling time
3s 8.625 MPa 30 s
956 Dent Mater J 2011; 30(6): 954–959

was calculated to the nearest 0.01%. For each polymer
blend material, the mean value of five test specimens
was calculated.
Statistical analysis
All recorded values were analyzed using a statistical
software (SPSS v.15.0, SPSS Inc., Chicago, IL, USA).
Data are presented as mean value±standard deviation in
Tables 2–5. One-way ANOVA was used to determine the
presence of statistically significant differences between
different polymer blend materials and commercial
thermoplastic products.
RESULTS
Tear strength
Tables 2–4 show the tear strength and elongation at
break results of PETG/PC, PETG/TPU, and PETG/PC/
TPU respectively.
When PETG was blended with PC, tear strength
increased with increasing blend ratio of PC but
elongation-at-break value decreased (Table 2). When
PETG was blended with TPU, elongation-at-break value
increased with increasing blend ratio of TPU but tear
strength decreased (Table 3). At the blending ratio of
70/10/20 for PETG/PC/TPU, optimal values were
reached: tear strength was 50.23 MPa and elongation at
break was 155.99% (Table 4). At this blending ratio,
there were no statistically significant differences between
PETG/PC/TPU and Erkodur or Biolon (p>0.05).
Stress relaxation rate
Tables 2–4 show the stress relaxation rates of PETG/PC,
PETG/TPU, and PETG/PC/TPU respectively.
When PETG was blended with PC, stress relaxation
rate increased with increasing blend ratio of PC (Table
2). When PETG was blended with TPU, stress relaxation
rate decreased with increasing blend ratio of TPU (Table
3). At the blending ratio of 70/10/20, stress relaxation
rate of PETG/PC/TPU was 0.0136 N/s after 1 hour, which
was slower than Erkodur and Biolon (p=0.024 and 0.018)
(Table 4).
Water absorption rate
Table 5 shows the water absorption behaviors of the
different blending ratios of PETG/PC/TPU at different
immersion times in comparison with Erkodur and
Biolon. During the first 48 hours of immersion, water
absorption rate was rather high for both the commercial
products and PETG/PC/TPU at all blending ratios. This
was followed by a slowdown and eventually a plateau
after 2 weeks of immersion.
Despite a general trend in water absorption behavior
for the tested materials over a 2-week immersion period,
it was observed that the water absorption rate of PETG/
PC/TPU increased with an increase in TPU blending
ratio. At 2 weeks, there were no statistically significant
differences between the blending ratios of 80/10/10 and

Table 2 Comparison of mechanical properties of PETG/PC at different blending ratios (n=5, x±s)
PETG/PC Tear strength (MPa) Elongation at break (%) Stress relaxation rate (N/s)
100/ 0 45.12 (2.15)a 141.22 (4.85)a 0.0192 (0.0005)ab
90/10 52.94 (2.44) b
111.65 (4.11) ab
0.0266 (0.0009)ab
80/20 54.33 (2.31)b 105.21 (3.84)ab 0.0288 (0.0006)ab
60/40 59.63 (2.05) ab
  94.93 (3.81) ab
0.0301 (0.0006)ab
40/60 61.54 (2.91)ab   86.62 (3.47)ab 0.0356 (0.0008)ab
Erkodur 54.62 (2.56) 150.16 (5.26) 0.0148 (0.0006)
Biolon 48.56 (2.85) 145.22 (4.94) 0.0153 (0.0004)
a
Significantly different from Erkodur by one-way ANOVA (p<0.05).
b
Significantly different from Biolon by one-way ANOVA (p<0.05).

Table 3 Comparison of mechanical properties of PETG/TPU at different blending ratios (n=5, x±s)
PETG/TPU Tear strength (MPa) Elongation at break (%) Stress relaxation rate (N/s)
100/0 45.12 (2.15) a
141.22 (4.85) a
0.0192 (0.0005)ab
95/5 44.25 (2.32)ab 148.88 (5.15) 0.0181 (0.0005)ab
90/10 44.01 (2.02) ab
151.62 (5.31) b
0.0168 (0.0007)ab
85/15 43.25 (2.18)ab 157.61 (5.77)ab 0.0151 (0.0003)
80/20 42.52 (2.07) ab
158.72 (5.62) ab
0.0131 (0.0005)ab
Erkodur 54.62 (2.56) 150.16 (5.26) 0.0148 (0.0006)
Biolon 48.56 (2.85) 145.22 (4.94) 0.0153 (0.0004)
a
Significantly different from Erkodur by one-way ANOVA (p<0.05).
b
Significantly different from Biolon by one-way ANOVA (p<0.05).
 Dent Mater J 2011; 30(6): 954–959 957

Table 4 Comparison of mechanical properties of PETG/PC/TPU at different blending ratios (n=5, x±s)
PETG/PC/TPU Tear strength (MPa) Elongation at break (%) Stress relaxation rate (N/s)
80/10/10 52.83 (2.55) b
135.25 (3.82) ab
0.0172 (0.0004)ab
70/10/20 50.23 (2.43) 155.99 (5.65) ab
0.0136 (0.0002)ab
60/10/30 47.07 (2.57)a 169.31 (6.85)ab 0.0121 (0.0006)ab
50/10/40 42.77 (2.31)ab 171.37 (6.41)ab 0.0113 (0.0003)ab
40/10/50 34.98 (1.85) ab
182.57 (7.13) ab
0.0098 (0.0002)ab
Erkodur 54.62 (2.56) 150.16 (5.26) 0.0148 (0.0006)
Biolon 48.56 (2.85) 145.22 (4.94) 0.0153 (0.0004)
a
Significantly different from Erkodur by one-way ANOVA (p<0.05).
b
Significantly different from Biolon by one-way ANOVA (p<0.05).

Table 5 Comparison of water absorption rates of PETG/PC/TPU at different blending ratios (% weight increase)
PETG/PC/TPU 6h 12 h 24 h 48 h 168 h 336 h
80/10/10 0.15 (0.013)ab 0.18 (0.019)ab 0.28 (0.027)ab 0.40 (0.047)ab 0.51 (0.026)ab 0.52 (0.021)ab
70/10/20 0.12 (0.014)ab 0.22 (0.021)ab 0.33 (0.033)ab 0.42 (0.031)ab 0.53 (0.033)ab 0.57 (0.023)ab
60/10/30 0.17 (0.016)ab 0.23 (0.015)ab 0.30 (0.031)ab 0.51 (0.058)ab 0.64 (0.021)ab 0.67 (0.024)ab
50/10/40 0.12 (0.011)ab
0.21 (0.026) ab
0.31 (0.026) ab
0.51 (0.023) ab
0.67 (0.028) ab
0.72 (0.026)ab
40/10/50 0.14 (0.017)ab 0.21 (0.031)ab 0.29 (0.028)ab 0.53 (0.021)ab 0.72 (0.036)ab 0.73 (0.035)ab
Erkodur 0.34 (0.021) 0.43 (0.044) 0.58 (0.017) 0.72 (0.037) 0.76 (0.029) 0.80 (0.027)
Biolon 0.33 (0.025) 0.45 (0.015) 0.58 (0.023) 0.73 (0.020) 0.78 (0.018) 0.81 (0.015)
a
Significantly different from Erkodur by one-way ANOVA (p<0.05).
b
Significantly different from Biolon by one-way ANOVA (p<0.05).

70/10/20 (p=0.992). However, there were significant
differences between the blending ratios of 80/10/10 and
70/10/20 and the other three blending ratios (p<0.05).
When compared with the commercial products, PETG/
PC/TPU at 70/10/20 blending ratio exhibited 0.57%
water absorption rate after 2 weeks, which was
significantly lower than Erkodur and Biolon (p=0.002
and 0.001).
DISCUSSION
Thermoplastic polymers are used as structural materials
in the fabrication of clear orthodontic appliances. In the
mouth, orthodontic appliances are subjected to both
short-term and long-term loading forces27). For example,
a short-term load is encountered when an orthodontic
appliance is fitted over a patient’s teeth. The appliance
may undergo severe deformation during fitting, but a
clear orthodontic appliance responds in an elastic
manner by returning to its original shape after the
short-term loading force causing the deformation is
removed. Once fitted over the patient’s teeth, the
appliance is subjected to long-term loading forces exerted
intermittently upon it between meals and when worn
overnight.
Though subjected to long-term loading in the mouth,
a clear thermoplastic appliance should nonetheless exert
continuous, controlled, orthodontic forces on teeth to
bring about tooth movement. Therefore, it is critically
important to have a thorough understanding of the effect
of long-term loading on the mechanical properties of
thermoplastic polymers. This helps to assess if a
particular thermoplastic material could fulfill the
purpose of an orthodontic appliance in providing light,
sustained orthodontic forces9) to accomplish effective
tooth movement. A thermoplastic material is viscoelastic
in nature, which means that the force generated by the
programmed movement decreases as a function of time.
Therefore, we seek a thermoplastic material that exhibits
substantial linear elastic behavior with a high yield
point.
Polyester, polyurethane, and polypropylene are the
dominant thermoplastic materials used in the fabrication
of clear orthodontic appliances. Amongst which, PET is
a widely used thermoplastic material because it has good
creep properties, fatigue resistance, and dimensional
stability10). However, our preliminary study revealed
that the mechanical properties of PET were inferior to
two commercial thermoplastic products, Erkodur and
Biolon. To improve the mechanical properties of PET,
styrene-ethylene-butylene-styrene block copolymer
(SEBS) and ethylene-propylene-diene monomer (EPDM)
were blended with PET to produce a polymer blend.
Blending modification yielded a polymer blend with an
opaque appearance and a lower rebound resilience. Both
characteristics did not meet the criteria for invisible
958 Dent Mater J 2011; 30(6): 954–959
orthodontic appliances.
PETG is a modified product of PET, which has good
mechanical properties, formability, fatigue resistance,
and dimensional stability10-12). However, results of this
study showed that the tear strength and elongation-at-
break value of PETG were 45.12 MPa and 141.22%
respectively, which were inferior to Erkodur and Biolon.
In our preliminary study, PC, TPU, PMMA, and
polyethersulfone (PES) were selected to improve the
mechanical properties of PETG. However, the blends of
PETG/PMMA and PETG/PES turned out opaque.
Therefore, only PC and TPU were used in this study to
improve the mechanical properties of PETG.
Results of this study showed that the tear strength
of PETG/PC increased with blending ratio of PC, but
elongation at break decreased. Stress relaxation rate
became faster with increase in PC blending ratio. These
results indicated that with increase in PC blending ratio,
short-term elastic recovery increased, but long-term
performance reliability decreased. Conversely, the tear
strength of PETG/TPU decreased as the blending ratio of
TPU increased, but elongation at break increased. Stress
relaxation rate became slower as the blending ratio of
TPU increased. These results thus indicated that with
increase in TPU blending ratio, long-term performance
reliability increased but short-term elastic recovery
decreased.
When the blending ratio of PETG/PC was 90/10,
tear strength was 52.94 MPa —which was close to that of
Erkodur’s at 54.62 MPa. Proffit28) stated that the ideal
orthodontic forces are 0.35–0.60 N. Hahn et al.29)
reported that the forces delivered by Erkodur were 3 to
11 times higher than the ideal forces. Barbagallo et al.30)
revealed that Erkodur exerted a high level of force
against the tooth to be moved at the initial stage followed
by a rapid force diminish. Taken together, it could be
assuredly claimed that PETG/PC of 90/10 blending ratio
could deliver sufficient force against the tooth to be
moved. However, elongation at break at this blending
ratio was 111.65%, which was significantly lower than
Erkodur (p=0.001). On the other hand, stress relaxation
rate was 0.0266 N/s, which was significantly higher than
Erkodur (p=0.014). Taken together, these results
suggested that this blend could not provide sufficient,
sustainable orthodontic forces during treatment and
that elasticity of blend should be improved.
Pure TPU is a ductile elastomer, which might aid in
improving the elasticity of PETG/PC polymer blend.
Therefore, if the blends were well compatibilized, both
ultimate elongation and tensile strength could be
improved. Keeping the blending ratio of PC at 10%,
increase in TPU blending ratio brought about a decrease
in the tear strength of PETG/PC/TPU, an increase in
elongation at break, and a slower stress relaxation rate.
When the blending ratio of PETG/PC/TPU was 70/10/20,
optimal properties were exhibited: tear strength was
50.23 MPa, elongation at break was 155.99%, and stress
relaxation rate was 0.0136 N/s after 1 hour —which was
slower than Erkodur and Biolon. These results indicated
that this PETG/PC/TPU polymer blend could provide
sufficient and more sustainable orthodontic forces during
treatment than Erkodur and Biolon.
Water may react chemically with the polymer
backbone chain through a process called hydrolysis. Due
to water absorption, several physicochemical changes
take place in the material, causing the mechanical
properties of the polymer to be irreversibly degraded31-33).
Hence, moisture in any form is unfriendly for polymers
as it often causes swelling and degradation34). For
example, an in vitro study found that water absorption
induced dimensional changes in numerous commercial
mouth guard products, which had compositions similar
to those of thermoplastic overlay orthodontic materials35).
In the mouth, dimensional changes due to hygroscopic
expansion may affect the fit of appliances fabricated
from these thermoplastic materials, causing changes to
orthodontic forces delivered by these appliances. For
these reasons, an ideal thermoplastic material for
orthodontic appliances should have low water absorption
property.
In the present study, the water absorption rate of
PETG/PC/TPU increased with blending ratio of TPU. At
70/10/20 blending ratio, water absorption rate was 0.57%
after 2 weeks, which was lower than Erkodur and Biolon.
These results implied that aligners fabricated using this
PETG/PC/TPU blend would have greater dimensional
stability than Erkodur and Biolon, since water would
have little adverse influence on the mechanical properties
of PETG/PC/TPU polymer blend as compared to Erkodur
and Biolon.
ACKNOWLEDGMENTS
This study was supported by The Key Laboratory of
Beijing City on Preparation and Processing of Novel
Polymer Materials.
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