Clin Oral Invest
DOI 10.1007/s00784-014-1272-8
ORIGINAL ARTICLE
Color stability of adhesive resin cements after immersion in coffee
Maho Shiozawa & Hidekazu Takahashi & Yuya Asakawa &
Naohiko Iwasaki
Received: 27 January 2014 / Accepted: 9 June 2014
# Springer-Verlag Berlin Heidelberg 2014
Abstract
Objectives Marginal discoloration of luting cement may af-
fect the appearance of esthetic restorations. This study evalu-
ated the color stability of current adhesive resin cements after
immersion in coffee.
Materials and methods Four dual-cured resin cements
(Clearfil SA cement Automix Universal, Maxcem Elite
Clear, Maxcem Elite Yellow, and RelyX Unicem2 Automix
A2) and two chemical-cured resin cements (Super-Bond C&B
Clear and Super-Bond C&B Esthetic) were examined. The
CIE L*a*b* of 2.0-mm-thick disc-shaped specimens was
measured using a spectrophotometer on a white background
(n=6). The color differences (ΔE) after 1-day and 1-week
immersion in 37 °C water or coffee were analyzed by two-
way ANOVA by selecting immersion solution and product as
main factors, followed by Tukey’s HSD test (α=0.05). Water
sorption and solubility were also evaluated.
Results The two-way ANOVA of the ΔEs suggested that the
two main factors and their interaction were significant. The
ΔEs after coffee immersion were significantly greater than
those after water immersion, except for Super-Bond C&B
Esthetic. The ΔEs after water immersion were not significant-
ly different among the products; those of Maxcem Elite Clear
and Maxcem Elite Yellow after coffee immersion were
M. Shiozawa
Removable Partial Prosthodontics, Department of Masticatory
Function Rehabilitation, Division of Oral Health Sciences, Graduate
School, Tokyo Medical and Dental University, 1-5-45 Yushima,
Bunkyo-ku, Tokyo 113-8549, Japan
H. Takahashi (*) : Y. Asakawa : N. Iwasaki
Oral Biomaterials Engineering, Course for Oral Health Engineering,
School of Oral Health Care Sciences, Faculty of Dentistry, Tokyo
Medical and Dental University, 1-5-45 Yushima, Bunkyo-ku,
Tokyo 113-8549, Japan
e-mail: takahashi.bmoe@tmd.ac.jp
significantly greater than the others. The water sorption and
solubility significantly correlated with the ΔEs.
Conclusions The ΔEs of the adhesive resin cements examined
after 1-week coffee immersion were significantly different
among the products. The product showing greater water sorp-
tion and solubility displayed greater color change.
Clinical relevance Adhesive resin cements should be careful-
ly selected when the marginal appearance of the ceramic
restoration is important.
Keywords Adhesive resin cements . Color stability . Water
sorption . Water solubility
Introduction
Ceramic restorations such as all-ceramic crowns, porcelain
laminate veneers, and ceramic inlays and onlays are popular
due to their esthetic appearance. Adhesive resin cements are
the material of choice for the luting of ceramic restorations
because of their excellent esthetics and good mechanical
properties such as flexural strength, compressive strength,
and shear and tensile bond strength [1–3]. The adhesive nature
of the resin cements promotes superior retention and fracture
resistance of the restorations [4–6]. The adhesive resin ce-
ments are categorized based on bonding procedure and/or use:
total etch, bond, plus resin; one-step etch-bond, plus resin;
self-adhesive resin; and dual-affinity adhesive resin [2]. These
cements are also categorized by polymerization type:
chemical-cured, light-cured, and dual-cured [2, 4, 5].
Recently, dual-cured adhesive resin cements have often been
selected for luting because of their ability to self-cure under
restorations [7]. Dual-cured adhesive resin cements can be
hardened in deep areas or beneath restorations where the
curing light cannot penetrate, while they can also be

polymerized by the curing light at the restoration margins for
easy removal of excess cement [5].
Because adhesive resin cements at the restoration margins
are exposed to the oral environment, discoloration of resin
cements is caused by not only intrinsic but also extrinsic
factors. Intrinsic factors are material-related factors such as
the composition of the resin matrix [8] and filler [9], the
loading and particle size distribution of the filler, the type of
photoinitiator [10] and polymerization systems [11], and the
conversion ratio of the carbon-carbon double bonds [12];
these intrinsic factors are accelerated by UV irradiation [13]
or thermal change [12]. Extrinsic factors are stains caused by
food components, beverages, and smoking; these factors are
modulated by the conversion ratio and physicochemical char-
acteristics of the resin cements, such as water sorption rate
[14] and surface roughness [15].
Discoloration of the adhesive resin cements affects the
esthetic appearance of ceramic restorations. Marginal discol-
oration of ceramic inlays and onlays increases with time due to
the color changes in adhesive resin cements [16]. Therefore,
these cements need to have sufficient color stability to maintain
good esthetics. Adhesive resin cements usually contain an
adhesive functional monomer consisting of hydrophilic and
hydrophobic functional groups. Hydrophilic functional groups
are considered to possess higher water sorption [7, 17, 18], and
thus, they undergo greater color change. However, the color
stability of current adhesive resin cements after immersion in
discoloring media has not been clearly elucidated.
Many investigations evaluated the color stability of resin-
based composite materials in a variety of beverages such as
coffee [8, 9, 13, 14, 19–25], black tea [8, 11, 13, 14, 19,
22–25], red wine [8, 9, 11, 13, 22–25], and cola [8, 19, 20,
22–25]. These beverages are common in people’s daily diet
and are reported to have the potential to stain restorative
materials. The results of these experiments showed that the
color changes were generally greater in red wine, coffee, and
tea compared to cola [19, 8, 23, 24]. Coffee is considered to be
one of the beverages with a higher potential to stain [8].
The objective of the present study was to evaluate the color
stability of current adhesive resin cements after immersion in
coffee. The null hypothesis was that the immersion solution
and the type of adhesive resin cements had no influence on the
color change of adhesive resin cements.
Materials and methods
Materials and immersion solution
The four dual-cured adhesive resin cements and two
chemical-cured adhesive resin cements evaluated in the pres-
ent study are listed in Table 1; four cements were tooth-
colored and two were transparent. Their compositions are
Clin Oral Invest
listed in Table 2. They were prepared at 23±2 °C according
to each manufacturer’s instructions. The dual-cured type was
prepared using the light-curing mode. The chemical-cured
type was prepared using the bulk-mix technique.
Color stability measurement
Disc-shaped specimens (10 mm in diameter and 2.1 mm thick)
were prepared in an acrylic mold (n=6). The dual-cured
specimens were polymerized with a light-emitting diode
(LED) light-curing unit (Elipar S10, 3 M ESPE, Seefeld,
Germany) with light intensity of 1,200 mW/cm2 for 40 s on
each side. The chemical-cured-type specimens were polymer-
ized in an incubator at 37±2 °C for 1 h. The specimens were
ground sequentially using a series of SiC grinding sheets
(#600, 1,000, and 1,500). The grinding and polishing proce-
dures were performed on one side of the specimens to make
2.0-mm-thick specimens. The final thickness was checked
with a digital micrometer (MDC-25 M, Mitsutoyo, Tokyo,
Japan) having an accuracy of ±0.01 mm. Before each mea-
surement, the specimens were ultrasonically cleaned in dis-
tilled water for 10 min and dried with compressed air. Each
specimen was immersed in distilled water at 37±2 °C for 24 h
in a 100-mL brown glass vial. Before performing the colori-
metric measurements, the specimens were removed from the
vials and washed with distilled water, gently wiped with filter
paper, and dried by shaking in air for 30 s.
The CIE L*a*b* values of the polished surfaces of each
specimen were measured on a white glossy photo paper
(KA420PG, Seiko Epson Corp., Nagano, Japan): L*=91.57,
a* = −1.02, and b* = 1.56 using a spectrophotometer
(Crystaleye, Olympus Corp., Tokyo, Japan) [26]. Prior to data
acquisition, the spectrophotometer was calibrated using a
calibration plate and positioned at a consistent distance of
16 mm from the specimen surface using the special contact
cap for object measurement. The light source illumination of
seven-band LED lights corresponding to average daylight
(D65) was irradiated at a 45° angulation, and the diffusion
refraction light was measured. The color difference (ΔE) was
obtained by calculating the color difference between the spec-
imen before and after immersion in one of the solutions using
the following equation:
h i1=2
ΔE ¼ ðL1 −L2 Þ2 þ ða1 −a2 Þ2 þ ðb1 −b2 Þ2
where L* refers to the brightness, a* for redness to greenness,
and b* for yellowness to blueness. The subscripts 1 and 2 refer
to the color coordinates before and after immersion, respec-
tively. A high ΔE value indicates great color difference. Three
measurements were taken for each specimen, and the average
value was recorded.
Clin Oral Invest

Table 1 Adhesive resin cements investigated

Product Code Shade Polymerization type Filler content (wt%)a Lot no. Manufacturer

Clearfil SA Cement Automix CSA Universal Dual-cured 66 056AAA Kuraray Noritake

Dental Inc.
Maxcem Elite MEC Clear Dual-cured 69 4438232 Kerr Corp.
Maxcem Elite MEY Yellow Dual-cured 69 4772310 Kerr Corp.
RelyX Unicem 2 Automix RXU A2 Dual-cured 70 463439 3 M ESPE
Super-Bond C&B SBC Clear Chemical-cured 0 Monomer: FX1, catalyst: Sun Medical Co.
FM43F, powder: FX31
Super-Bond C&B SBE Esthetic Chemical-cured 0 Monomer: FX1, catalyst: Sun Medical Co.
FM43F, powder: FW1
a
Claimed by the manufacturer

Two types of immersion solution were prepared: distilled
water and coffee solution. The coffee solution was prepared
by dissolving 0.51 g of instant coffee powder (Nescafe Gold
Blend, Nestle Japan, Kobe, Japan) in 50 mL of distilled water
[9]. Six specimens of each resin cement were immersed in one
of the immersion solutions in a shaking incubator (37±2 °C,
1 Hz frequency). The immersion solution was changed every
day. The color measurements were taken after 1-day and 1-
week immersion.
Water sorption and solubility
The water sorption and solubility of each resin cement
were determined according to ISO 4049:2009. Disc-shaped
specimens (15 mm in diameter and 1 mm thick) were
prepared using a metal mold (n=5). The dual-cured-type
specimen was exposed to overlapping irradiation with the
LED light-curing unit for 40 s on each side and then
stored in the incubator at 37±2 °C for 15 min. The
chemical-cured-type specimen was polymerized in the in-
cubator at 37±2 °C for 1 h. The specimens were removed
from the mold and kept in a desiccator maintained at 37±
2 °C. After 22 h, the specimens were removed and stored
in another desiccator kept at 23±2 °C for 2 h and then
weighed using a precision digital balance (AUW120D,
Shimadzu, Kyoto, Japan; the minimum reading is
0.01 mg). This cycle was repeated until a constant mass
was obtained, i.e., until the mass loss of each specimen
was not more than 0.1 mg in any 24-h period. The
diameter and height of each specimen were measured to
calculate the volume. The specimens were immersed in
distilled water at 37 °C for 1 week, then removed, gently
dried with filter paper, and weighed again. The specimens
were returned to the desiccators using the above-

Table 2 Compositions of adhesive resin cements

Code Base resin Filler Other

CSA Paste A 10-Methacryloyloxydecyl dihydrogen phosphate Silanated barium glass filler, silanated dl-Camphorquinone, benzoyl
(MDP), Bis-GMA, TEGDMA, hydrophobic colloidal silica peroxide, initiator
aromatic dimethacrylate
Paste B Bis-GMA, hydrophobic aromatic dimethacrylate, Silanated barium glass filler, silanated Accelerators, pigments, surface-
hydrophobic aliphatic dimethacrylate colloidal silica treated sodium fluoride
MEY Base paste Urethane dimethacrylate Fluoroalminosilicate glass Camphorquinone
MEC Catalyst paste Bis-GMA, glycerol dimethacrylate, glycerol Barium aluminoborosilicate glass
phosphate dimethacrylate
RXU Base paste Methacrylate monomers containing phosphoric Silanated fillers Initiator components, stabilizers,
acid groups, methacrylate monomers rheological additives
Catalyst paste Methacrylate monomers Alkaline (basic) fillers, silanated fillers Initiator components, stabilizers,
pigments, rheological additives
SBE Catalyst Tri-n-butylborane (TBB), acetone
SBC Monomer Methyl-methacrylate, 4-methacryloxyethyl
trimellitate anhyderide (4-META)
Polymer Polymethyl-methacrylate Pigments (esthetic)

Bis-GMA bis-phenol A diglycidylmethacrylate, TEGDMA triethyleneglycol dimethacrylate


mentioned procedure until a constant mass was obtained.
The water sorption and solubility were calculated using
the following equations:
Water sorption ¼ ðm2 −m3 Þ=V
Water solubility ¼ ðm1 −m3 Þ=V
where m1 is the mass obtained after the specimen was initially
dried (μg); m2 is the mass after the period of immersion in
water (μg); m3 is the final mass after the specimen was dried
(μg); and V is the initial volume of each specimen (mm3).
Filler content
The inorganic filler content of each specimen was measured
using the standard ash method according to ISO 1172:1996.
An alumina crucible (PC2, Nikkato, Osaka, Japan) was held
in an electric furnace (Auto Furnace QF1, GC Corp., Tokyo,
Japan) set at 625 °C for 30 min. After cooling to ambient
temperature in the desiccator, the weight of the crucible was
measured until a constant mass was obtained. A droplet of the
resin cement (approximately 0.1 g, n=3) was inserted in the
crucible, and the weight of each specimen including the
crucible was measured with the precision digital balance.
The specimen and crucible were then heated in the electric
furnace at 625 °C for 30 min to burn out the organic matrix.
After cooling to ambient temperature in the desiccator, the
residue and crucible were reweighed until a constant mass was
obtained. The inorganic filler content (wt%) was determined
using the following equation:
Filler content ¼ ðm3 −m1 Þ=ðm2 −m1 Þ  100
where m1 is the initial mass of the dry crucible (g); m2 is the
initial mass of the dry crucible plus the dried specimen (g); and
m3 is the final mass of the crucible plus the residue after
calcination (g).
Morphological observation
The polished surfaces of the specimens were observed using a
scanning electron microscope (SEM) to evaluate the filler
morphology. Disc-shaped specimens (4 mm in diameter and
2 mm thick) were prepared using a Teflon mold according to
the same procedure described for the color measurement
experiment. The specimens were embedded in an acrylic resin
(Palapress Vario, Heraeus Kulzer, Hanau, Germany). The
surface of the specimens was polished with sheets of SiC
paper (1,000, 1,500, and 2,000 grit) and 0.06-μm Al2O3
suspensions. The specimens were ultrasonically cleaned,
dried, mounted on aluminum stubs, and then coated with
Clin Oral Invest
carbon. Three randomly selected areas of the specimen surface
were observed using a scanning electron microscope (S-4500,
Hitachi High-Technologies Corp., Tokyo, Japan).
Statistical analysis
The color differences (ΔE) after immersion were analyzed by
two-way analysis of variance (ANOVA) by selecting the
immersion solution and product as the main factors using
JMP software (version 9.0, SAS Institute, Cary, NC, USA).
Tukey’s honestly significant difference test was used to com-
pare the individual data. The level of significance was set at
α=0.05.
Results
The specimens after immersion in coffee became darker in
color as the immersion period increased; the MEC and MEY
specimens in particular showed greater color changes.
However, the color changes of the specimens after water
immersion were not perceptible by visual observation.
Table 3 shows the L*, a*, and b* values and the means and
standard deviations of the color differences after immersion
for 1 day and 1 week. The ΔE values after coffee immersion
greatly increased as the immersion period increased, but those
after water immersion only slightly increased. Two-way
ANOVA revealed that the two main factors, immersion solu-
tion and product and their interaction, were significant. The
ΔE values after coffee immersion for 1 day for MEC, MEY,
and RXU were significantly greater than those after water
immersion; the ΔE values after coffee immersion for 1 week
were significantly greater than those after water immersion
except for SBE. The ΔE values after water immersion were
not significantly different among the products, while the ΔE
values after coffee immersion of MEY and MEC were signif-
icantly greater than those of the others; the ΔE of MEC was
significantly greater than that of MEY. Regarding the coffee
solution immersion, the L* value decreased with an increase
of the immersion period, but the a* and b* values increased
regardless of the product. Regarding SBC and SBE after water
immersion, the b* value slightly increased with an increase of
the immersion period, but the L* and a* values did not
change.
The means and standard deviations for the water sorption
and solubility are shown in Table 4. The water sorption and
solubility displayed a similar tendency. MEC and MEY
showed greater water sorption and solubility values com-
pared to the other products. The water solubility value
of RXU was negative.
The filler contents of the adhesive resin cements are sum-
marized in Table 5. The dual-cured-type cements contained
Clin Oral Invest

Table 3 Color difference (ΔE) after immersion in distilled water and coffee solution for 1 day and 1 week

Polymerization type Code Water Coffee

Start 1 day 1 week Start 1 day 1 week

Dual-cured CSA L* 82.9 82.6 81.8 82.8 80.9 78.8

a* 1.1 1.3 1.6 1.2 1.8 2.3
b* 25.4 25.6 25.6 25.9 26.4 27.3
ΔE 0.5 (0.1)d,e,f 1.3 (0.2)b,c 2.4 (1.2)D,E 4.8 (2.1)D
MEC L* 86.8 86.8 87.0 86.9 77.0 69.7
a* −1.9 −1.9 −1.8 −2.1 0.7 4.1
b* 2.5 2.7 2.6 2.5 19.7 25.8
ΔE 0.3 (0.2)e,f 0.5 (0.3)d,e,f 20.1 (3.1)B 29.7 (2.4)A
MEY L* 78.8 78.9 79.4 79.0 76.7 73.7
a* 1.9 2.0 1.7 1.7 2.7 4.1
b* 25.3 25.5 25.1 24.8 28.4 32.4
ΔE 0.2 (0.1)f 0.7 (0.2)d,e,f 4.5 (0.8)D 9.6 (1.4)C
RXU L* 80.2 80.1 80.3 80.4 78.7 77.7
a* 1.9 1.9 1.4 1.7 2.6 2.8
b* 21.2 21.5 21.7 21.4 23.2 24.8
ΔE 0.4 (0.1)e,f 0.8 (0.3)d,e 2.6 (0.2)D,E 4.5 (0.8)D
Chemical-cured SBC L* 90.3 90.1 90.0 90.1 89.4 88.5
a* −2.0 −2.3 −2.7 −2.1 −2.3 −2.6
b* 1.0 1.9 3.1 1.1 3.4 5.4
ΔE 0.9 (0.4)c,d 2.3 (0.4)a 2.4 (0.3)D,E 4.7 (0.3)D
SBE L* 79.2 79.2 79.3 79.3 78.3 77.9
a* 6.3 6.1 5.9 6.4 6.4 6.5
b* 21.8 22.6 23.3 22.1 23.3 24.4
ΔE 0.9 (0.2)c,d 1.5 (0.3)b 1.6 (0.1)E 2.7 (0.2)D,E

Standard deviations are in parentheses, and the same superscript letter denotes homogenous subsets (p>0.05)

63.6–68.2 wt% of inorganic filler; however, a trace of inor-
ganic filler was found in the chemical-cured-type cements.
These results corresponded with the filler content claimed by
the manufacturer except for RXU, which was smaller than
manufacturer claimed value. This discrepancy might be due to
using the standard ash method.
SEM images of representative areas of the specimens
are displayed in Fig. 1. The size of inorganic filler
particles was largest in CSA, approximately 70 μm,
followed by MEC and MEY. Pre-polymerized filler par-
ticles were found in CSA. No inorganic filler particles
were observed in SBC and SBE, but partially dissolved
crushed poly(methyl methacrylate) (PMMA) particles
were seen.
Figures 2 and 3 showed the relationships among the
water sorption and solubility and the color differences
after 1-week coffee and water immersion, respectively.

Table 4 Water sorption and solubility after water immersion for 1 week
(μg/mm3) Table 5 Filler content of adhesive resin cements (wt%)

Polymerization type Code Water sorption Water solubility Polymerization type Code Filler content

Dual-cured CSA 6.4 (0.1) 0.3 (0.0) Dual-cured CSA 64.6 (0.3)
MEC 16.0 (0.2) 2.5 (0.3) MEC 68.2 (0.1)
MEY 12.0 (0.1) 1.1 (0.1) MEY 67.9 (0.1)
RXU 7.9 (0.2) −0.8 (0.1) RXU 63.6 (0.1)
Chemical-cured SBC 7.1 (0.2) 0.2 (0.2) Chemical-cured SBC 0.1 (0.1)
SBE 7.2 (0.1) 0.1 (0.0) SBE 0.1 (0.2)

Fig. 1 SEM images of adhesive
resin cement surface
The ΔE after coffee immersion significantly correlated
with both the water sorption and solubility (p=0.006
and 0.01), but those after water immersion did not
(p=0.12 and 0.39).
Discussion
The dual-cured adhesive resin cements evaluated in the pres-
ent study were self-adhesive resin cements, which have been
advertised as bonding to the tooth structure without any pre-
treatment. Several in vitro studies reported promising results
with respect to dentin bond strength compared to resin-
modified glass ionomer cements and conventional resin ce-
ments [27–30].
Luting cements at the restoration margins are usually ex-
posed to the oral environment. In the present study, marginal
discoloration of the dual-cured and chemical-cured resin ce-
ments caused by intrinsic and extrinsic factors was simulated.
The physical properties of dual-cured adhesive resin cement
Fig. 2 Relationship between water sorption and color difference after 1-
week immersion. r2 with * was statistically significant (p<0.05)
Clin Oral Invest
have been reported to vary, depending on the curing mode
[31]. The dual-cured type cements at the restoration margins
are usually polymerized by the curing light for easy removal
of excess cement. Therefore, the dual-cured-type cements in
the present study were prepared using the light-curing mode.
The color difference will be increase when the oxygen
inhibited layer is present on the specimen surface. However,
measured surface was polished and the oxygen inhibited layer
did not exist on the specimen surface in the present study. In
clinical situation, the oxygen-inhibited layer might exist and
this layer would be more stained compared to the results of the
present study.
The adhesive resin cement is used to place a restoration on
the tooth. Therefore, the white background was selected in the
present study. The color difference after coffee immersion
greatly increased as the immersion period increased, but those
after water immersion only slightly increased. This tendency
was similar to the results of previous studies of resin-based
composite materials [8, 23, 24]. The two-way ANOVA
Fig. 3 Relationship between water solubility and color difference after 1-
week immersion. r2 with * was statistically significant (p<0.05)
Clin Oral Invest
revealed that the two main factors, immersion solution and
product, and their interaction were significant. The null hy-
pothesis that the immersion solution and the type of adhesive
resin cements had no influence on the color change of adhe-
sive resin cements was rejected. The color differences after
coffee immersion were different among the products. The
coffee solution caused greater color changes to MEC and
MEY.
The products that underwent greater color change resulted
in greater water sorption and solubility. In the present study,
six adhesive resin cements containing an adhesive functional
monomer with hydrophilic functional groups were selected.
The color difference after coffee immersion of adhesive resin
cements was greater compared to that of composite resins
containing no adhesive functional monomer [9, 13, 20].
According to the results in the present study, adhesive func-
tional monomer might responsible for greater color change.
The thickness of the specimen for the color measurement
was 2.0 mm due to its handling and intention to reduce the
background effect. However, the thickness of the specimen for
the water sorption measurement was 1.0 mm according to ISO
4049. If the thickness of the water sorption specimen was
2.0 mm, surface area and amount of water sorption would
increase, but the required time until saturation would be
extended. However, the tendency of the water sorption among
tested products would be the same regardless of the thickness
of the specimen.
Water sorption is mostly due to absorption in the resin
matrix [23]. The composition and content of the resin matrix
and the bond strength of the resin-filler interface influence the
degree of water sorption. Greater water sorption causes the
expansion and plasticizing of the resin, which creates micro-
cracks. As a result, food and beverage stains penetrate into the
micro-cracks or the interfacial gaps between the resin and
filler, causing the discoloration [23]. Therefore, the product
that showed higher water sorption produced greater color
change after coffee immersion. The brown colorant of cof-
fee, which is reported to be due to the water-soluble
polymer compounds produced during the roasting proce-
dure [32], might be absorbed and adsorbed into the resin
matrix, resin-filler interface, and micro-cracks on the ce-
ment surface. The filler particle size and composition of
the resin matrix and filler were different among the prod-
ucts. There was no obvious relationship between the filler
content and the color difference after coffee immersion.
SBC and SBE contained only PMMA filler, which was
dissolved by the resin monomer MMA. The resin-filler
interface was tightly sealed. This might be a reason why
SBC and SBE had smaller color changes compared to the
other products.
Several investigations evaluated the perceptibility and ac-
ceptability threshold for color differences of dental materials
in CIELAB color space [33–36]. The color perceptibility and
acceptability threshold varied among the reports. The ΔE
value of perceptibility for dental composite veneer restora-
tions and tooth substance was 3.7 [33]. The ΔE values of color
perceptibility and acceptability threshold for denture teeth
were 2.6 and 5.5, respectively [34]; those for dental ceramics
were 1.8 and 3.5, respectively [35]; and those for denture teeth
were 1.9 and 4.2, respectively [36]. In the present study, ΔE
values after 1-week water immersion, which were less than
2.3, were smaller than previously reported acceptability
threshold, while those after 1-week coffee immersion of
MEC and MEY were greater than the previously reported
acceptability threshold of 5.5. Furthermore, other studies re-
ported individual thresholds for the L*, a*, and b* directions
[37] or L, C, and H directions [38]. There were no significant
differences between perceptibility and acceptability thresh-
olds, which were 1.25 in the a* and L* directions and 2.8 in
the b* direction [37]. In the present study, ΔL*, Δa*, and Δb*
values of all products after 1-week water immersion were less
than perceptibility and acceptability thresholds. After 1-week
coffee immersion, ΔL* values of all products were greater
than 1.25; Δa* values of MEC and MEY were greater than
1.25; and Δb* values of all products except for CSA and SBE
were greater than 2.8. The color difference after coffee im-
mersion might be recognized by the change of brightness, the
ΔL* value.
One week of coffee immersion was considered to simulate
about 1 year of coffee drinking, with the assumption that one
cup of coffee is consumed for 30 min each day. Moreover, the
coffee manufacturer reports that the average time for con-
sumption of one cup of a drink among coffee drinkers is
15 min, and the average consumption of coffee is 3.2 cups
per day [25]. Based on this data, 1-week coffee immersion
might simulate 7-month coffee drinking if coffee solution
constantly remained in the mouth during drinking. Because
actual contact time of coffee with oral tissues during drinking
is shorter, 1-week coffee immersion probably simulated lon-
ger than 7-month coffee drinking. After 1-week coffee immer-
sion, adhesive resin cements evaluated in the present study
showed great color change, which was considered clinically
unacceptable. Therefore, discoloration of adhesive resin ce-
ments with time would be a clinical problem. These resin
cements should be used where the restoration margin
does not cause esthetic problems, e.g., beneath the gin-
gival margin.
In the present in vitro study, the effect of 1-week coffee
and water immersion on the color stability of adhesive
resin cements was evaluated. However, tooth brushing or
thermal cycling effects were not simulated. Therefore, the
limitation of the present study is that the clinical perfor-
mance of the adhesive resin cements examined was not
evaluated. Future studies are needed to evaluate the effects
of these factors on the long-term color stability of adhesive
resin cements.

Conclusion
Within the limitations of the experimental methods employed
in the present study, the following conclusions can be drawn:
1. The color differences after coffee immersion were signif-
icantly greater than those after water immersion, except
for SBE.
2. The color differences after water immersion were not
significantly different among the products. The ΔE values
of MEY and MEC after coffee immersion were signifi-
cantly greater than those of the others; the ΔE of MEC
was significantly greater than that of MEY.
3. The color differences after coffee immersion significantly
correlated with the water sorption and solubility. The
products with greater water sorption and solubility
displayed greater color change.
4. The color difference after coffee immersion did not show
obvious correlation with the filler content.
5. The color differences after coffee immersion for 1 week
were considered to be clinically acceptable (ΔE < 5.5)
except for MEC and MEY.
Acknowledgments The authors would like to thank Professor
Motohiro Uo, Advanced Biomaterials of Tokyo Medical and Dental
University (TMDU), for his valuable suggestions.
Conflict of interest The authors declare that they have no conflict of
interest.
References
1. Rosenstiel SF, Land MF, Crispin BJ (1998) Dental luting agents: a
review of the current literature. J Prosthet Dent 80:280–301
2. Hill EE, Lott J (2011) A clinically focused discussion of luting
materials. Aust Dent J 56(Suppl 1):67–76
3. Ladha K, Verma M (2010) Conventional and contemporary luting
cements: an overview. J Indian Prosthodont Soc 10:79–88
4. Blatz MB, Sadan A, Kern M (2003) Resin-ceramic bonding: a review
of the literature. J Prosthet Dent 89:268–274
5. Haddad MF, Rocha EP, Assunção WG (2011) Cementation of pros-
thetic restorations: from conventional cementation to dental bonding
concept. J Craniofac Surg 22:952–958
6. Bindl A, Lüthy H, Mörmann WH (2006) Thin-wall ceramic CAD/
CAM crown copings: strength and fracture pattern. J Oral Rehabil
33:520–528
7. Marghalani HY (2012) Sorption and solubility characteristics of self-
adhesive resin cements. Dent Mater 28:e187–e198
8. Arocha MA, Mayoral JR, Lefever D, Mercade M, Basilio J, Roig M
(2013) Color stability of siloranes versus methacrylate-based com-
posites after immersion in staining solutions. Clin Oral Investig 17:
1481–1487
9. Imamura S, Takahashi H, Hayakawa I, Loyaga-Rendon PG,
Minakuchi S (2008) Effect of filler type and polishing on the discol-
oration of composite resin artificial teeth. Dent Mater J 27:802–808
10. Schneider LF, Pfeifer CS, Consani S, Prahl SA, Ferracane JL (2008)
Influence of photoinitiator type on the rate of polymerization, degree
Clin Oral Invest
of conversion, hardness and yellowing of dental resin composites.
Dent Mater 24:1169–1177
11. Falkensammer F, Arnetzl GV, Wildburger A, Freudenthaler J (2013)
Color stability of different composite resin materials. J Prosthet Dent
109:378–383
12. Shin DH, Rawls HR (2009) Degree of conversion and color stability
of the light curing resin with new photoinitiator systems. Dent Mater
25:1030–1038
13. Stober T, Gilde H, Lenz P (2001) Color stability of highly filled
composite resin materials for facings. Dent Mater 17:87–94
14. Um CM, Ruyter IE (1991) Staining of resin-based veneering mate-
rials with coffee and tea. Quintessence Int 22:377–386
15. Gönülol N, Yilmaz F (2012) The effects of finishing and polishing
techniques on surface roughness and color stability of nanocompos-
ites. J Dent 40(Suppl 2):e64–e70
16. Santos MJ, Mondelli RF, Navarro MF, Francischone CE, Rubo JH,
Santos GC Jr (2013) Clinical evaluation of ceramic inlays and onlays
fabricated with two systems: five-year follow-up. Oper Dent 38:3–11
17. Ito S, Hashimoto M, Wadgaonkar B, Svizero N, Carvalho RM, Yiu C,
Rueggeberg FA, Foulger S, Saito T, Nishitani Y, Yoshiyama M, Tay
FR, Pashley DH (2005) Effects of resin hydrophilicity on water sorp-
tion and changes in modulus of elasticity. Biomaterials 26:6449–6459
18. Yiu CK, King NM, Carrilho MR, Sauro S, Rueggeberg FA, Prati C,
Carvalho RM, Pashley DH, Tay FR (2006) Effect of resin hydrophi-
licity and temperature on water sorption of dental adhesive resins.
Biomaterials 7:1695–1703
19. Malekipour MR, Sharafi A, Kazemi S, Khazaei S, Shirani F (2012)
Comparison of color stability of a composite resin in different color
media. Dent Res J (Isfahan) 9:441–446
20. Bayindir F, Kürklü D, Yanikoğlu ND (2012) The effect of staining
solutions on the color stability of provisional prosthodontic materials.
J Dent 40(Suppl 2):e41–e46
21. Park JK, Kim TH, Ko CC, García-Godoy F, Kim HI, Kwon YH
(2010) Effect of staining solutions on discoloration of resin nano-
composites. Am J Dent 23:39–42
22. Cörekçi B, Irgın C, Malkoç S, Oztürk B (2010) Effects of staining
solutions on the discoloration of orthodontic adhesives: an in-vitro
study. Am J Orthod Dentofacial Orthop 138:741–746
23. Ertaş E, Güler AU, Yücel AC, Köprülü H, Güler E (2006) Color
stability of resin composites after immersion in different drinks. Dent
Mater J 25:371–376
24. Bagheri R, Burrow MF, Tyas M (2005) Influence of food-simulating
solutions and surface finish on susceptibility to staining of aesthetic
restorative materials. J Dent 33:389–398
25. Guler AU, Yilmaz F, Kulunk T, Guler E, Kurt S (2005) Effects of
different drinks on stainability of resin composite provisional restor-
ative materials. J Prosthet Dent 94:118–124
26. Wang F, Takahashi H, Iwasaki N (2013) Translucency of dental
ceramics with different thicknesses. J Prosthet Dent 110:14–20
27. Sabatini C, Patel M, D’Silva E (2013) In vitro shear bond strength of
three self-adhesive resin cements and a resin-modified glass ionomer
cement to various prosthodontic substrates. Oper Dent 38:186–196
28. Hitz T, Stawarczyk B, Fischer J, Hämmerle CH, Sailer I (2012) Are
self-adhesive resin cements a valid alternative to conventional resin
cements? A laboratory study of the long-term bond strength. Dent
Mater 28:1183–1190
29. Lührs AK, Guhr S, Günay H, Geurtsen W (2010) Shear bond
strength of self-adhesive resins compared to resin cements with etch
and rinse adhesives to enamel and dentin in vitro. Clin Oral Investig
14:193–199
30. Aschenbrenner CM, Lang R, Handel G, Behr M (2012) Analysis of
marginal adaptation and sealing to enamel and dentin of four self-
adhesive resin cements. Clin Oral Investig 16:191–200
31. Ilie N, Simon A (2012) Effect of curing mode on the micro-
mechanical properties of dual-cured self-adhesive resin cements.
Clin Oral Investig 16:505–512
Clin Oral Invest
32. Borrelli RC, Visconti A, Mennella C, Anese M, Fogliano V (2002)
Chemical characterization and antioxidant properties of coffee
melanoidins. J Agric Food Chem 50:6527–6533
33. Johnston WM, Kao EC (1989) Assessment of appearance match by
visual observation and clinical colorimetry. J Dent Res 68:819–822
34. Douglas RD, Steinhauer TJ, Wee AG (2007) Intraoral determination
of the tolerance of dentists for perceptibility and acceptability of
shade mismatch. J Prosthet Dent 97:200–208
35. Ghinea R, Pérez MM, Herrera LJ, Rivas MJ, Yebra A, Paravina RD
(2010) Color difference thresholds in dental ceramics. J Dent Suppl
2:e57–e64
36. Alhazali N, Burnside G, Moallem M, Smith P, Preston A,
Jarad FD (2012) Assessment of perceptibility and acceptabil-
ity of color difference of denture teeth. J Dent 40(Suppl 1):
e10
37. Lindsey DT, Wee AG (2007) Perceptibility and acceptability of
CIELAB color differences in computer-simulated teeth. J Dent 35:
593–599
38. Perez Mdel M, Ghinea R, Herrera LJ, Ionescu AM, Pomares H,
Pulgar R, Paravina RD (2011) Dental ceramics: a CIEDE2000 ac-
ceptability thresholds for lightness, chroma and hue differences. J
Dent 39(Suppl 3):e37–e44