CLINICAL SCIENCES

Color stability of denture base acrylic resins in three food colorants

Nur Hersek, DDS, PhD,a ~enay Canay, DDS, PhD, b Gfilay Uzun, DDS, PhD,c and Fatih Yildiz, PhD d
Faculty of Dentistry, University of Hacettepe, Ankara, Turkey
S t a t e m e n t o f p r o b l e m . Three commonly used artificial dyes in food technology are erythrosine, tar-
trazine, and sunset yellow.
Purpose. The color stability of 5 commercially available denture base acrylic resins (QC-20, Meliodent,
Trevalon, Trevalon High, and Lucitone) was studied in vitro.
M e t h o d s . The specimens were exposed to 3% erythrosine, tartrazine, and sunset yellow solutions at
23~ • I~ Color changes were determined with a computer-controlled spectrophotometer. Five speci-
mens from each material were processed, and initial color measurements were made after 1, 3, and 6 months
of exposure to the staining solutions. Finally, the color stability was quantitatively measured again, and color
differences (AE) were calculated.
Results. For the observations made in 1, 3, and 6 months intervals, the specimens that exhibited the least
color change were in the sunset yellow solution. The greatest color changes observed according to the
National Bureau of Standards unit system were Lucitone (2.71) in erythrosine solution, Lucitone (2.54),
QC-20 (1.71) in tartrazine solution, and QC-20 (1.66) in sunset yellow solution. The changes in the other
acrylic resins in the 3 solutions were slight and at trace level.
Conclusions. All materials tested were acceptable from the standpoint of color stability for long-term
exposure to these food colorants. (] Prosthet Dent 1999;81:375-9.)

CLINICAL IMPLICATIONS
In this study, Lucitone QC-20 acrylic resin specimens exhibited noticeable color change
or staining in compliance with the NBS unit system. Staining in Meliodent, Treval-
on, and Trevalon High acrylic resins were at slight or trace levels. As the frequency of
ingestion a n d contact of the erythosine, tartrazine, and sunset yellow food colorants
with dentures was limited to only a few minutes a day, it is unlikely the colorants can
stain clean acrylic resin surfaces.

Amost all complete dentures are fabricated by
using an acrylic resin, a low cost material that requires
relatively easy manipulation and construction methods.
However, it is not the ideal material in every respect.
Discoloration o f acrylic resins results in esthetic prob-
lems, and a denture base polymer should have good
esthetics with a smooth and glassy surface and be capa-
ble o f matching the natural appearance o f the soft tis-
sues. For the best esthetic effect, the material should be
translucent. Color and translucency should be main-
tained during processing, and these resins should not
get stained or change color in clinical use. The color
stability criteria may provide important information on
the serviceability o f these materials.1
aprofesso5 Department of Prosthodontics.
bAssociate Professor, Department of Prosthodontics.
CAssistant, Department of Prosthodontics.
dprofessor, Department of Food Engineering, University of Middle
EastTechnical University, Ankara.
Most materials used for prosthetic treatment are
subject to sorption, a process o f absorption and adsorp-
tion o f liquids dependent on environmental conditions.
Should a contacting solution be pigmented, discol-
oration is possible. 2 Polymethyl methacrylate absorbs
water slowly over time. 3 Discoloration o f the denture
base polymers may be caused by the oxidation o f the
amine accelerator or by the penetration o f colored solu-
tions. Many studies have been r e p o r t e d on discol-
oration characteristics o f resin-based dental restorative
materials. 4-8 Color changes o f denture base materials
during exposure to oral fluids, and denture cleaners
have been reported. T M There is evidence that bever-
ages such as tea, coffee, and wine significantly increase
the development o f stain on enamel and acrylic resin.
However, there is no report on discoloration o f den-
ture base materials in food colorants. Three commonly
used food colorants, erythrosine, tartrazine, and sunset
yellow, were used to measure discoloration o f dentures.
These 3 dyes are used in beverages, beverage powders,
jellies, jams, candies, puddings, ice cream, and many

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THE JOURNAL OF PROSTHETIC DENTISTRY
Table I. Acrylic resin materials used in this study
Materials Manufacturer
QC-20 De Trey Division, Dentsply Ltd,
Weybridge, Surrey, U.K.
Meliodent
Bayer UK Ltd, Newberry, Berkshire,
U.K.
Trevalon De Trey Division, Dentsply Ltd
Trevalon HI De Trey Division, Dentsply Ltd
Lucitone De Trey Division, Dentsply Ltd
other food formulations. These colorants are used at a
0.1% to 0.3% level in foods and are highly soluble in
water. Because they have electrostatic charges on their
structures, they may stain surfaces.
Co!orimetry is a branch of color science and is based
on the digital expression of the color perceived from
the object. In assessing chromatic differences, 2 color
systems are used: Munsell color system and standard
Commission Internationale de L' Eclairage (CIE Lab)
color system. The American Dental Association (ADA)
recommends the use of the CIE Lab color differential
system. According to this system, all colors in nature
are obtained through the blending of 3 basic colors,
namely, red, blue, and green in certain proportions.
The CIE Lab system has been developed on the basis
of this system. In examining various materials with
regard to color, this technique is also being used quite
extensively by researchers in dentistry. 12-1s In fact,
instruments of colorimetry that can be used intraorally
have been recently developed. 16
Color stability is a required characteristic of denture
base resins, as specified by various national and interna-
tional standards and may provide important informa-
tion on the serviceability of these materials.Lll There-
fore the purpose of this study was to determine the
color stability of 5 denture base acrylic resins by sub-
jecting them to 3 solutions used in food technology.
MATERIAL AND METHODS
In this study, 5 brands of acrylic resin materials, 2
high-impact and 3 conventional heat-cured denture
base acrylic resins, were examined (Table I). Specimens
were prepared in rectangular blocks (20 x 10 x 1.5 mm
dimensions) in a plastic mold to meet the demands of
the measuring instrument. Fifteen specimens were
made for each material studied. They were allowed to
undergo short-time polymerization in a water bath at
72~ for 1.5 hours, followed by 30 minutes boiling in
100~ water. After being processed, the specimens
were abraded on both sides with 600-grit silicon-car-
bide paper to a final thickness of 1.5 + 0.1 mm, which
is regarded as the most inappropriate clinical situation
of surface roughness. The specimens were first divided
into 3 groups for each test solution, then for each solu-
376
HERSEK ET AL
tion 5 specimens were coded, from 1 to 5, on the back
of the specimens.
Dyes that are frequently used in the coloring of food,
3% V / W erythrosine, tartrazine, and sunset yellow solu-
tions, were prepared by dissolving 3 g of dye in 100 mL
of distilled water (Table II). Solutions prepared were
poured into sealable 200-mL jars and 5 specimens were
placed in each jar. The specimens were then stored in
3 solutions for a 6-month period at 23~ + I~
Five specimens of the same acrylic resin were com-
pletely immersed in each solution. They were placed
together to avoid specimen-to-specimen contact.
Experimental recordings were taken before immersion
and after 1, 3, and 6 months of exposure to staining
solutions. Before any recordings were obtained, all
specimens were removed from the solutions and rinsed
in distilled water. Excess water on the surfaces was
removed with tissue paper and the specimens were
allowed to dry. After initial measurements, specimens
were placed in glass jars and stored in the dark at room
temperature. During each test, color measurements of
all specimens were repeated.
Color measurements were made in 3 randomly
selected areas by using an ultraviolet-visible recording
spectrophotometer (Model UV-2100, Shimadzu,
Kyoto, Japan). The average of the 3 readings were
recorded and the mean of each material was calculated
with the use of the CIE Lab uniform color scale. Color
characteristics of 5 specimens for each denture base
material were compared by a white standard. This was
a pressed powder tablet of barium-sulfate. The magni-
tude of the total color difference is formulated by a sin-
gle number AE:
AE = [(AL*) 2 + (Aa*) 2 + (Ab*)2] 5
where L* stands for lightness, a* for redness-greenness,
and b* for yellowness-blueness. This formula is
designed to provide numeric data that represents the
magnitude of the color difference perceived in between
2 objects. A total of 900 recordings were taken from 75
blocks. To determine the average color change after 1,
3, and 6 months, the mean and standard deviation of
the 5 materials for each solution were calculated. The
effects of the solution on the acrylic resin due to time
were compared.
Statistical analysis was conducted. The significance
of the color changes exhibited by the acrylic resins in 3
solutions were compared for equal lengths of time with
the Mann-Whitney U test. The significance of the color
changes exhibited by each acrylic resin specimen kept
for different lengths of time in the same solution were
also compared with the Mann-Whitney U test.
RESULTS
In the CIE LAB color system, AE value signifies the
combination of differences in the 3 dimensions of the
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HERSEK ET AL THE JOURNAL OF PROSTHETIC DENTISTRY

Table II. Dyes used in the study

Dyes Code no. Chemical name and formula

Erythrosine FD&C red no. 3 Xanthine

Universal Food Corp, Disodium salt o f 9-o-carboxyphenyl-6-hydoxy-2,4,5,7-tetraiodo-3-isoxanthione
Lynwood, III.
Tartrazine FD&C yellow no. 5 Pyrazolone
Universal Food Corp Trisodium salt of 3-carboxy-5-hydrozy-l-p-sulfophenyl-4-p-sulphophenylazo-pyrazole
Sunset yellow FD&C yellow no. 6 Monoazo
Universal Food Corp Disodium salt o f 1-p-sulfophenylazo-2-naphthol-6-sulfonic acid

Table III. The mean values and standard deviations (SD) of the color change (DE) of acrylic resins in erythrosine, tartrazine,
and sunset yellow solutions
QC 20 Meliodent Travalon Trevalon HI Lucitone

Erythrosine
Initial 57.09 + 1.04 63.46 + 1.17 57.28 • 0.83 60.97 + 1.36 59.34 + 1.77
30 days 56.49 + 0.68 63.20 + 1.15 53.30 • 1.30 60.10 + 0.56 59.81 + 2.09
90 days 56.54 + 2.30 62.99 • 0.55 57.30 + 1.04 60.66 • 1.11 57.68 • 2.04
180 days 55.66 • 0.96 62.30 • 1.98 57.93 • 0.87 59.56 • 0.72 56.38 • 0.98
Tartrazine
Initial 57.08 • 2.22 64.31 • 2.43 57.92 • 1.04 60.16 • 1.25 59.56 • 1.34
30 days 57.08 • 2.09 63.52 • 0.73 58.38 • 0.66 61.54 • 1.01 59.07 • 1.79
90 days 56.91 • 1.56 63.71 • 1.51 56.29 • 0.93 60.11 • 1.47 58.15 • 2.52
180 days 55.22 • 1.21 63.05 • 0.96 57.32 • 1.79 59.73 • 2.17 56.79 • 1.97
Sunset yellow
Initial 56.75 • 0.29 63.52 • 0.38 57.78 • 1.32 62.16 • 1.31 59.77 • 2.48
30 days 56.52 • 2.32 63.61 • 0.29 57.32 • 0.47 60.90 • 1.92 60.88 • 1.84
90 days 56.53 • 1.08 63.48 + 1.49 57.52 • 1.62 61.27 + 1.31 59.55 + 2.25
180 days 54.94 • 1.20 62.50 + 1.30 56.90 • 1.11 62.32 • 2.58 58.70 • 5.54

color space. The total color difference (DE) of the den-
ture base materials after 6 months of immersion in the
staining solutions are presented in Table III. The
results show that Lucitone produced slightly larger
color changes than the others in erythrosine and tar-
trazine solutions. The least color change was observed
in sunset yellow solution.
As a result of the comparison of samples of the same
kind of acrylic resin in 3 solutions for the same period,
the difference between the initial and first month AE
values in tartrazine and sunset yellow solutions of
Trevalon was found to be significant (P=.016). On the
other hand, the difference in initial and first month AE
values in erythrosine and tartrazine solutions of Treval-
on HI was also found to be significant (P=.028). In
others the difference was statistically insignificant.
As a result of the comparison of the initial, first, third,
and sixth month results of each acrylic resin, the initial-
sixth month comparison of QC-20 in erythrosine
solution was significant (P=.05), and comparison of the
differences between initial and third months (P=.05),
and first and third months (P=.014) of Trevalon in tar-
trazine solution was also statistically significant. Howev-
er, for Lucitone in erythrosine and tartrazine solutions,
the initial-sixth month comparisons were also significant
(P=.016 and P=.05, respectively). Differences between
all other groups were insignificant.
All materials showed only minor color changes, but
Trevalon and Trevalon HI materials exhibited good
color stability values in 3 and 2 solutions, respectively
(AE <1), whereas the other acrylic resin specimens
showed a visually perceptible color change in 3 solu-
tions. The critical remark of color change (AE) has
been quantified by the National Bureau of Standards
(NBS) with NBS units of color differences. NBS units
are expressed with the following formula:
NBS unit = AE*ab x 0.92
Table IV presents the critical remarks of color differ-
ences when the mean AE values of the specimens were
converted to NBS units. From this conversion, Treval-
on HI specimens exhibited a trace difference in tar-
trazine and sunset yellow solutions and slight staining
in erythrosine solution. Slight staining was demonstrat-
ed for Lucitone specimens only in sunset yellow solu-
tion and QC-20 specimens in erythrosine solution,
along with Meliodent and Trevalon specimens in all 3
solutions. Noticeable staining was observed with Luci-

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Table IV. The color change values after 6 months according to the National Bureau of Standards unit system
Solution QC-20 Meliodent
Erythrosine 1.31 * 1.06*
Tartrazine 1.71 + 1.15*
Sunset yellow 1.66 f 0.93*
Critical remarks of color difference:
Trace (0.0-0.5);
*Slight (0.5-1.5);
tNoticeable (1.5-3.0).
tone samples in erythrosine, QC-20 and Lucitone sam-
pies in tartrazine, and QC-20 samples in sunset yellow
solution.
DISCUSSION
CIE Lab system is a tmiform 3-dimensional system
that determines color changes. It is widely used in
determining chromatic differences and is more advan-
tageous than Munsell color system. In this system, the
3 dimensions of color have been arranged at almost
equal intervals. Through the evaluation of color differ-
ences that express various combinations of differences
in 3 dimensions of color space, mathematical data are
obtained. This system was preferred for our study. In
this study, spectrophotometric measuring techniques
were used to determine the color of 5 types of acrylic
resin in 3 test media. Color was expressed in terms of
CIE Lab color coordinates.
When color changes of denture base resins with
respect to solutions were studied, the least staining was
found to be in the sunset yellow solution. The 3 food
colorants used in this study have charged and ionizable
groups in their chemical structures. They were water
soluble azo dyes and stable with heat, alkalis, and acids.
The polymethyl methacrylate denture base resins were
hydrophilic that attracted more water soluble dyes on
the surface and staining, which occurs as a result of
electrostatic charges. All 5 resins used in this study had
the same base chemical structures; however, each of
them contained small quantities of different cross-
linking agents, and plasticizers, pigments, which may
explain the difference in staining properties
(hydrophilicity) of resins. There also seemed to be
some molecular interactions between colorants and
denture polymers that resulted in slight discoloration in
acrylic resins. Erythrosine (MW = 879.9) and tartrazine
(MW = 534.4) have 3 electrostatically charged groups
on the molecule when ionized; however, sunset yellow
contains 2 ionizable groups in the molecule, which may
explain why it did not stain as much as the other 2 dyes.
The NBS parameter is important for color compari-
son. When the results were evaluated according to the
NBS units of color difference, Lucitone exhibited the
378
HERSEK ET AL
Acrylic resin
Trevalon Trevalon HI Lucitone
0.59* 1.29* 2.71 t
0.56* 0.4 2.54 t
0.80* 0.15 0.99*
greatest chromatic change (2.71) for erythrosine solu-
tion. Lucitone (2.54) and then QC-20 (1.71), exhibit-
ed the greatest change in tartrazine solution, and
QC-20 in sunset yellow solution (1.66) at noticeable
grades (Table IV). Johnson and Kao 14 observed that, if
AE is less than 1, this chromatic value is deemed to be
slight and between 1 and 2, and the situation is clini-
cally acceptable. Goldstein and Schmitt16 reported that
when AE is more than 3.7, it is no longer within the
limits of clinical acceptability, and it assumes the quali-
ty of visual detectability. In our study, except for Luci-
tone, which exhibited the greatest staining in erythro-
sine and tartrazine solutions (AE = 2.96 and 2.77
respectively), the color changes exhibited by all speci-
mens after the sixth month are at clinically acceptable
levels. This excessive staining observed with Lucitone
may be related to the rubber phase in its structure. 17
The resin specimens absorbing these colorant solutions
also may undergo staining. The absorption is undoubt-
edly due primarily to the polar properties of resin mol-
ecules. However, it has been proven that the mecha-
nism is diffusion of water molecules that penetrate
according to the laws of diffusion. The diffusion coef-
ficient of a heat-cured denture acrylic resin is reduced
by one half when the temperature drops from 37~ to
23~ for these reasons, the diffusion coefficient may
be lower than the in vivo environment. 18
The aim of this study was to provide the lacking
research on the staining effect of food colorants on
denture materials, because current studies concentrate
on the staining effects of tea and coffee. Biiyiikyilmaz
and Ruyter19 demonstrated that after 1000 hours of
immersion in coffee and tea solutions, coffee produced
a higher discoloration value AE than tea. Brushing and
moderate grinding showed acceptable discoloration
values below 3.3 AE and they concluded that discol-
oration results from the adhesion of colorants to the
surface. 19 The effect of tannic acid, which is present in
tea and coffee, caused the staining.
In this study, the effect of the food stains was exam-
ined in a saliva- and diet-free medium; however, the
actual oral environment is comparatively different
because of the pellicles formed by the proteins and glu-
VOLUME 81 NUMBER 4
 HERSEK ET AL
coproteins in saliva that lead to the formation of plaque
adhering to the dentures. These soft materials are
affected by the dyes in food more quickly and undergo
color changes. 20
CONCLUSIONS
The results of this study indicated that the adhesive
that exhibited noticeable color change on specimens
were Lucitone, which exhibited the greatest chromatic
change in erythrosine solution, and in descending
order, Lucitone and QC-20 in tartrazine solution, and
QC-20 in sunset yellow solution.
The staining effect of the 3 food colorants on the 5
commercially available acrylic resins used as denture
base material were found to be at clinically acceptable
levels.
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Reprint requests to:
DR NUR HERSEK
BAGISSOKAK17/I 0
0660 KOCATEPE
ANKARA
TURKEY
FAX: 90-312-4184715
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Dentistry.
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