Dental Materials (2006) 22, 560–568

www.intl.elsevierhealth.com/journals/dema

The effects of common errors on sealing ability

of total-etch adhesives
Masanori Hashimotoa,*, Franklin R. Tayb, Nadia R. Svizeroc, Anton J.
de Geed, Albert J. Feilzerd, Hidehiko Sanoe, Masayuki Kagaa, David
H. Pashleyf
a
Division of Pediatric Dentistry, Hokkaido University, Graduate School of Dental Medicine, Kita 13, Nishi 7,
Kita-ku, Sapporo 060-8586, Hokkaido, Japan
b
Paediatric Dentistry and Orthodontics, Faculty of Dentistry, University of Hong Kong, Hong Kong SAR,
China
c
Department of Operative Dentistry, University of Sacred Heart, Bauru, SP, Brazil
d
Department of Dental Materials Sciences, Academic Centre for Dentistry Amsterdam (ACTA), Universiteit
van Amsterdam and Vrije Universiteit, Amsterdam, The Netherlands
e
Division of Cariology and Endodontology, Graduate School of Dental Medicine, Hokkaido University, Japan
f
Department of Oral Biology and Maxillofacial Pathology, School of Dentistry, Medical College of Georgia,
USA

Received 27 January 2005; received in revised form 22 May 2005; accepted 16 June 2005

KEYWORDS Summary Objectives: This study evaluated the effect of errors commonly made in
Air-drying; using total-etch adhesives, on the resulting bond strength, fluid movement and
Solvent removal; nanoleakage of resin dentin bonds.
Water permeability; Methods: Two total-etch adhesives were used for bonding to dentin according to the
Microtensile bond manufacturers’ recommendations, with meticulous solvent evaporation (control), or
strength; with the introduction of common bonding errors—wet bonding without solvent
Nanoleakage evaporation (no evaporation), and dry bonding.
Results: The 24-hour bond strength of the control was significantly higher than the
other groups (p !0.05). For all groups, the higher initial permeability declined
significantly after 24 h. The fluid movement across bonded dentin was similar in the
control and dry bonding for both adhesives, whereas significantly higher permeability
(p!0.05) was recorded for the no evaporation groups even after 24 h. Extensive
silver impregnation within hybrid layers was seen by TEM in the no evaporation and
dry bonding specimens after 24 h. Dry bonding caused collapse of the collagen matrix
and interfered with resin infiltration. In contrast, inadequate solvent evaporation
and/or residual water during dentin bonding results in dilution or incomplete
polymerization of the resin, leading to severe nanoleakage formation.
Significance: Increased permeability associated with incomplete solvent

* Corresponding author. Tel.: C81 11 706 4292, fax: C81 11 706 4307.
E-mail address: masanori-h@mue.biglobe.ne.jp (M. Hashimoto).

0109-5641/$ - see front matter Q 2005 Published by Elsevier Ltd on behalf of Academy of Dental Materials. All rights reserved.
doi:10.1016/j.dental.2005.06.004
The effects of common errors on sealing ability of total-etch adhesives 561

evaporation in total-etch adhesives may lead to poor bond strength.

Q 2005 Published by Elsevier Ltd on behalf of Academy of Dental Materials. All rights
reserved.

Introduction evaluate microtensile bond strengths, water per-

The use of contemporary total-etch adhesives
involves a degree of technique sensitivity that
may compromise bonding efficacy and marginal
seal of these adhesives [1,2]. Excessive air-drying
and incomplete adhesive solvent removal are
common errors associated with wet bonding on
vital dentin [3]. The air-drying of acid-etched
dentin (dry bonding) prevents optimal resin infiltra-
tion within the demineralized collagen network [4,
5]. Water has the highest solubility parameter for
hydrogen bonding among polar resin solvents [6,7].
Water molecules form hydration clusters around
the functional groups on collagen peptides [8–10]
and proteoglycans [11], resulting in the full
expansion of interfibrillar spaces that are used for
permeation of resin monomers. Conversely, inter-
peptide or peptide-proteoglycan hydrogen bonding
that develops during air-drying causes collapse of
interfibrillar spaces in the demineralized matrix
[12–15]. Incomplete evaporation of solvents results
in dilution [16,17], poor polymerization [18], or
phase separation of the resin components [19].
Recent total-etch adhesives contain high concen-
trations of water or organic solvents [20,21]. After
light-curing of the adhesives, residual water or
solvents may become pathways for water move-
ment within the hybrid or resin layers [22,23],
increasing the permeability of the resin-dentin
interfaces [24], and their subsequent susceptibility
to degradation via resin hydrolysis [25,26] and
collagen degrading enzymes [27,28]. Although
both bonding efficacy and the seal of bonded dentin
may be compromised by excessive air-drying or
incomplete solvent evaporation, it is not known
whether these variables are affected to the same
extent by these two common errors of wet bonding.
Therefore, the purpose of this study was to
meability and nanoleakage of resin-dentin bonds
made with two total-etch adhesives, using the wet
bonding technique, versus the two common errors
of wet bonding. The null hypothesis tested was that
there are no differences in bonding and sealing
under the conditions of excessive air-drying or
incomplete solvent removal.
Materials and methods
Test teeth
Unerupted, caries-free human third molars were
collected after the patients’ informed consent had
been obtained under a protocol reviewed and
approved by the Human Assurance Committee of
the Medical College of Georgia, Augusta, Georgia,
USA. The teeth were stored in thymol-saturated
isotonic saline at 4 8C to inhibit microbial growth,
and used within two months following extraction.
Each tooth was sectioned perpendicular to its
longitudinal axis using a diamond disk (Isomet,
Buehler Ltd., Lake Bluff, IL, USA) under water, to
expose a flat bonding surface in the mid-coronal
dentin. Each dentin surface was ground with 600-
grit silicon carbide paper under running water for
30 s just prior to bonding.
Test materials and bonding procedures
Two commercially available total-etch adhesives
(Excite/EX, Ivoclar Vivadent, Schaan, Liechtenstein
and OptiBond Solo Plus/OP, Kerr Corp., Orange, CA,
USA) were used in this study (Table 1). The
prepared dentin surfaces were acid-etched with
phosphoric acid (37% for EX and 37.5% for OP) for
15 s and then thoroughly washed using a water spray

Table 1 Compositions of the two simplified total-etch adhesives investigated.

Material (manufacturer) Etchant Adhesive
Excite (Ivoclar Vivadent, Schaan, 37% phosphoric acid gel Bis-GMA, HEMA, ethanol, water,
Liechtenstein) filler, CQ
OptiBond Solo Plus (Kerr Corp., 37.5% phosphoric acid gel Bis-GMA, GPDM, GDM, HEMA,
Orange, CA, USA) ethanol, water, filler, CQ
Bis-GMA, bisphenol A-glycigyl methacrylate; HEMA, 2-hydroxyethyl methacrylate; GPDM, glycerophosphate dimethacrylate; GDM,
glycerol dimethacrylate; CQ, dl-camphorquinone.
562
for 10 s. Three subgroups were designated for each
adhesive that differed in: (a) whether the acid-
etched dentin was left moist before adhesive
application, and (b) whether the adhesive solvent
was removed after adhesive application.
For the control groups, a wet bonding technique
was performed in which excess water was blot-
dried from the acid-etched dentin with an absor-
bent pellet, leaving the surface visibly moist. Each
adhesive was applied to the entire dentin surface
and the solvent was removed by gentle air-drying
for 10 s at a distance of 1 cm from the bonding
surface, to create a slightly shiny adhesive film.
Two consecutive coats of each adhesive were used
with solvent evaporation performed after the
application of each adhesive coat.
For the Dry Bonding subgroups, the acid-etched
dentin was intentionally air-dried for 10 s with oil-
free compressed air, by keeping the air syringe tip
at a distance of 1 cm away from the dentin surface.
Subsequent bonding procedures were conducted in
the same manner as the control groups, including
solvent evaporation. For the No Evaporation sub-
groups, bonding to the acid-etched was performed
via the wet bonding technique previously described
for the control groups. Two coats of adhesive were
also applied, but intentionally, without solvent
evaporation between the applications of each
adhesive coat. For each resin application, excess
adhesive resin was blot-dried from the dentin with
an absorbent pellet.
After the final application, the adhesive layer
was irradiated for 10 s with a light-curing unit
(Curing Light XL 3000, 3M ESPE, St Paul, MN, USA)
Figure 1 A schematic representation of the experimental setup employed in this study.
M. Hashimoto et al.
with a light output not less than 550 mW/cm2 for
all groups. Composite build-up was then per-
formed using five 1-mm thick increments of a
resin composite (AP-X; Kuraray Medical Inc.,
Osaka, Japan) that were individually light-cured
for 60 s.
Microtensile bond test
After the specimens were stored in distilled
water at 37 8C for 24 h, they were sectioned
perpendicular to the adhesive interfaces with the
diamond saw (Fig. 1) to produce resin-dentin
beams, each with an adhesive area of approxi-
mately 1.0 mm2. Three teeth were used for each
group and six to eight beams were obtained per
tooth, generating a total of 19–22 beams for
each group. The beams were then attached with
cyanoacrylate adhesive to a testing jig, and a
tensile load was applied with a universal testing
machine (Vitrodyne V1000, Chatillon, Green-
sboro, NC, USA) at a crosshead speed of
0.6 mm/min until failure to obtain the ultimate
tensile strength. The exact dimensions of each
tested beam were measured with a digital
micrometer (Sylvae Ultra-Cal 2, Fomuler Inc.,
Newton, MA, USA) after bond failure. Beams that
failed prematurely during specimen preparation
were assigned null bond strength values and
were included in the statistical analysis. The
bond strength data were evaluated by a two-way
ANOVA design (adhesive vs. bonding condition)
followed by Fisher’s PLSD multiple comparison
tests, with statistical significance set at pZ0.05.
The effects of common errors on sealing ability of total-etch adhesives
Evaluation of the permeability of adhesive-
bonded dentin
Seventy-two human third molars with bonding
surfaces in mid-coronal dentin were similarly
prepared by grinding the cut surfaces with 600-
grit SiC paper under running water. An additional
cut was made parallel to the bonding surface, using
the diamond saw under water cooling, to create
0.3 mm thick dentin disks, measured to the nearest
one-hundredth of a millimeter using the digital
micrometer. Twelve dentin disks were used for
each of the six groups.
The pulpal side of each dentin disk was acid-
etched with 37% H3PO4 for 15 s to remove the smear
layer, leaving the smear layer on the coronal
surface intact. After rinsing with water, the disk
was placed in a split-chamber [29]. Each disk was
bordered by identical rubber ‘O’-rings from the
upper and lower surfaces, giving a testing surface
area of 0.28 cm2 in dentin (Fig. 1). Fluid flow was
measured using an automated apparatus (Flodec,
DeMarco Engineering, Geneva, Switzerland) incor-
porating a glass capillary tube with an internal
diameter of 0.7 mm [30]. Fluid movement was
recorded by following the movement of an air
bubble created inside the capillary tube, using an
infrared beam that passed through one side of the
tube. A photosensitive diode, positioned on the
opposite side of the tube, detected any movement
of the air bubble. Permeability was calculated as:
PZ Jv/APt, where Jv Z fluid flow in mL, AZbonding
surface area in cm2, and tZtime in min. The
reduction in dentin permeability after dentin
bonding was expressed as a percentage of the
fluid flow through unbonded, acid-etched dentin
using the following equation: [water permeability
of resin-bonded dentin/water permeability of
unbonded acid-etched dentin] !100.
The experimental design involved measurements
of fluid flow under a physiological hydrostatic
pressure gradient [30] of 20 cm H2O for 6 min.
First, the coronal sides of the dentin disks were
etched with phosphoric acid (37% for EX and 37.5%
for OP) for 15 s without a simulated pulpal pressure
(0 cm H2O) and rinsed with water. Then the water
permeability was measured for 6 min with water
covering the top of the dentin to prevent any
evaporation fluid loss. After 6 min, the adhesives
were applied to the dentin within the split chamber
in a same manner as previously described. After
light-curing the adhesive for 10 s, about 10 mm3 of
a flowable resin composite (Protect Liner F, Kuraray
Medical Inc.) was placed on all of the resin-covered
dentin surfaces and then light-cured for 60 s.
563
Subsequently, the fluid flow of the resin-dentin
interface was re-measured for another 6 min at
20 cm H2O. The same measurement was also con-
ducted 24 h after bonding. Two-way ANOVA and
Fisher’s PLSD tests were used to compare fluid
movement for the six sub-groups of each adhesive
(i.e. control, dry-bonding and no evaporation at 0
and 24 h), with statistical significance set at pZ0.05.
Nanoleakage evaluation of TEM
Twelve additional 0.3 mm thick dentin disks were
similarly prepared. Two dentin disks were used for
each of the three subgroups within each adhesive
group, and were bonded in the manner as previously
described. After storing in distilled water at 37 8C
for 24 h, a 1 mm wide slab containing the resin-
dentin interface was prepared from the widest
portion of each bonded disk. Each slab was coated
with nail varnish that was applied 1 mm away from
the bonded interfaces. They were immersed in a
50 wt% ammoniacal silver nitrate tracer solution for
24 h, according to the silver impregnation protocol
for nanoleakage examination reported by Tay and
Pashley [22]. After reduction of the diamine silver
ions, the silver-impregnated slabs were processed
for TEM examination without demineralization.
Ninety nanometer thick, epoxy resin-embedded
sections were prepared and examined unstained
[22], using a TEM (CM100, Philips, Eindhoven, The
Netherlands) operating at 80 kV.
Results
Microtensile bond strengths
Fig. 2 represents the bond strength for the three
test groups (control, dry bonding, and no evapor-
ation). For both adhesives, the tensile bond
strengths of the control groups (EXZ50.0G
15.4 MPa; OPZ55.8G17.9 MPa) were significantly
higher (p !0.05) than those of the dry bonding
groups (EXZ11.9G10.8 MPa; OPZ3.6G5.3 MPa)
and the no evaporation groups (EXZ17.8G
14.5 MPa; OPZ12.3G9.1 MPa/OP).
Permeability of the bonded dentin
The percentage reductions in fluid flow through the
bonded dentin for the three Excite subgroups are
shown in Fig. 3A, and those for the OptiBond Solo
Plus subgroups in Fig. 3B. Similar trends were seen
with both adhesives. For all groups, the higher
initial permeability recorded for adhesive-bonded
564 M. Hashimoto et al.

Figure 2 Microtensile bond strength results (Means

(SD)) for each test group. Groups with bond strengths that
were significantly different (p!0.05) are indicated by
different letters above the bars. The number within the
bar represents the number of specimens tested for each
group.

dentin declined significantly (p!0.05) after 24 h.

The permeability to fluid movement were similar in
the Control and Dry Bonding subgroups using both
adhesives, whereas significantly higher fluid flow
(p!0.05) was recorded for the No Evaporation
subgroups, both immediately after bonding and
after 24 h. The highest fluid movements were
recorded immediately after bonding in the No
Evaporation subgroups (EXZ83.2G19.1%; OP Z
89.5G14.5%). No significant differences between
the Dry Bonding and Control subgroups were
observed immediately after bonding (pO0.05).
However, significant differences were seen
between the Dry Bonding and the Control subgroups
after 24 h (p!0.05).

Severity of nanoleakage Figure 3 Changes in the fluid movement across resin-

For the control wet bonding groups, both Excite
(Fig. 4A) and OptiBond Solo Plus (Fig. 5A) exhibited
minimal nanoleakage (i.e. silver uptake) that was
predominantly observed along the basal portions of
the 5 mm thick, completely demineralized hybrid
layers. Conversely, extensive nanoleakage was
observed within the hybrid layers in the No
Evaporation (Figs. 4B and 5B) and Dry Bonding
groups (Figs. 4C and 5C) of both adhesives. The
nanoleakage was so severe that each entire hybrid
layer was impregnated with silver deposits, with
those in the Dry Bonding groups probably resulting
from the re-expansion of the collapsed, resin-
sparse collagen matrix after immersion in 37 8C
water for 24 h. Extensive silver deposition was
additionally observed within the dentinal tubules,
and between the first and second adhesive coats in
bonded dentin of Excite (A), and OptiBond Solo Plus (B)
immediately after and 24 h after bonding. The values
were expressed as percentages of fluid flow across
unbonded acid-etched dentin (100%; control). Values
are Means (SD)). Groups that were significantly different
are indicated by different letters (nZ12 for each group).
the No Evaporation groups of both Excite (Fig. 4B)
and OptiBond Solo Plus (Fig. 5B). By contrast, the
dentinal tubules and adhesive layers were generally
devoid of silver deposition in the Dry Bonding groups
of the two adhesives.
Discussion
The bond strengths achieved following the appli-
cation of two consecutive adhesive coats with the
The effects of common errors on sealing ability of total-etch adhesives 565

Figure 5 TEM micrographs of the resin-dentin interface

Figure 4 TEM micrographs of the resin-dentin inter-
of OptiBond Solo Plus. C: composite; A: filled adhesive; D:
face of Excite, depicting the effect of common errors
mineralized dentin; H: hybrid layer. A. In the control,
of dentin bonding on silver deposition (nanoleakage). C:
reticular silver deposits (pointer) were only sporadically
composite; A: filled adhesive; D: mineralized dentin; H:
identified along the base of the completely demineralized
hybrid layer. A. In the control, nanoleakage of
hybrid layer (H). B. When wet bonding was performed
silver (pointer) could only be sporadically identified
without solvent evaporation, the entire demineralized
within the unstained, 5 mm thick hybrid layer (H).
collagen matrix (M) was filled with silver deposits. Silver
Nanofiller clusters (open arrowhead) were sparsely
deposits were also identified within the subjacent
distributed within the adhesive. B. When wet bonding
dentinal tubules (asterisk) and between the first and
was performed without solvent evaporation (No Evap-
second adhesive coats (open arrow). C. When specimens
oration group), the entire demineralized collagen
were bonded after air-drying of the acid-etched dentin,
matrix (M) and the subjacent dentinal tubules (asterisk)
the demineralized collagen matrix (M) was filled with
were heavily filled with silver deposits. A discontinuous
silver deposits. Filled adhesive could be observed within
band of silver (open arrow) was also observed
resin tags in the dentinal tubules (pointers).
between the first and second coat of adhesive. C.
With dry bonding, only the demineralized collagen wet bonding (controls over 50 MPa) were substan-
matrix (M) contained heavy silver deposits. Resin
tially higher than those achieved with either air-
tags completely filled the dentinal tubles. The unin-
filtrated collagen matrix probably collapsed on air- drying or incomplete solvent removal (below
drying, and re-expanded during immersion in the 20 MPa). This suggests that the bonding efficacy of
storage water. the total-etch adhesives were severely compro-
mised by these operator-dependent variables [31].
566
Although the hybrid layers in both the dry bonding
and no evaporation groups were heavily impreg-
nated with silver deposits, different mechanisms
are probably responsible for the nanoleakage. With
dry bonding, collapse of the interfibrillar spaces
resulted in a dense, collagen-rich matrix that was
almost completely devoid of resin infiltration. After
bonding, re-expansion of the resin-sparse, col-
lagen-rich matrix during immersion in the storage
water created normal interfibrillar spaces that
were filled with water rather than resin. When
these specimens were immersed in silver nitrate
solution, the tracer solution filled these water-filled
spaces where it was subsequently reduced to
metallic silver deposits. In specimens in the No
Evaporation subgroups, the interfibrillar spaces
contained residual water and adhesive solvents as
well as porous resin, that were subsequently
saturated with silver tracer solution. The lack of
resin infiltration within the collagen matrices is
thought to have resulted in the low bond strengths
observed in the Dry Bonding groups. The low bond
strengths in the No Evaporation groups was
probably a result of poor cross-linking and conver-
sion of the resin.
Similar to the results of previous studies [32–34],
a perfect seal of acid-etched dentin was not
realized in either of the control groups. Never-
theless, the reductions in permeability immediately
after bonding, and particularly at 24 h after bonding
in the current study were larger than those reported
for Excite and OptiBond Solo Plus (ca. 40%
reduction) by others [33]. The large differences in
measured flow rates between control vs. Dry
Bonding or No Evaporation groups argues against
any leakage around the edges of the ‘O’-rings within
the split chamber device. This enables valid
comparisons to be made among the permeability
results of the control and experimental groups.
The permeability of the resin-dentin interfaces
in the Dry Bonding groups were similar to the
control groups immediately after bonding, and
were only slightly less than those of the control
groups after 24 h. This is in sharp contrast to the
highly permeable interfaces in the No Evaporation
groups. The seal of the resin-dentin interfaces in
the Dry Bonding groups was compromised to a lesser
extent than the No Evaporation groups, as there
was better resin tag formation in the Dry Bonding
groups, apart from the differences in porosities of
the uninfiltrated collagen matrices (Figs. 4 and 5).
The authors believe that differences in the quality
of resin tags among the groups was responsible for
the large difference in permeability. Incomplete
solvent evaporation from the No Evaporation groups
in the present study, or the entrapment of water
M. Hashimoto et al.
within resin-dentin interfaces in dentin perfusion
studies [35], may result in dilution, incomplete
polymerization, and/or phase separation of the
adhesive resin tags, further increasing the per-
meability of the bonded dentin.
Although the wet bonding technique expands
acid-etched dentin matrix, the presence of this
water may inadvertently dilute the concentration
of adhesive monomers, thereby lowering their
inward rate of diffusion within the demineralized
collagen matrix. The water in interfibrillar spaces
can compete with the adhesive monomers for
binding sites on collagen [36]. The excess water
may also prevent optimal polymerization and cross-
linking of the adhesive monomers. Using a 62% Bis-
GMA/37% HEMA-based bonding agent, the effect of
increasing water concentration on the percent
conversion of double bonds, bond strength and
phase changes were reported by Jacobsen and
Söderholm [18]. As water was added to the bonding
agent, the percent conversion fell rapidly from
53.5% at 0% water, to 22.7% when 20% water was
added.
Phase separation of adhesive resin components
has been previously reported to occur [37],
particularly in simplified adhesive formulations
that contain hydrophobic resin components [38].
Spencer and Wang [19] further examined the
amount of water necessary to produce phase
changes in 70% BisGMA/30% HEMA formulation
solvated in 45% ethanol. This formulation exhibited
phase separations at 28 vol% water. If the formu-
lations were made of 30% BisGMA/70% HEMA
solvated in 45% ethanol, phase separations did not
occur until the water concentration reached 45%.
These factors, individually or in combination, could
have contributed to the large increase in the
permeability of the bonded interfaces when wet
bonding was performed without meticulous solvent
evaporation (i.e. No Evaporation subgroups).
The phenomenon of increased permeability
within resin-dentin interfaces was first reported in
simplified self-etch adhesives, and was manifested
morphologically as entrapment of fluid droplets
along the surface of the polymerized adhesives [39,
40]. Water movement through the hybrid layers and
adhesive layers [24,41–43] has subsequently been
reported for simplified total-etch adhesives that
lack the comparatively hydrophobic resins
employed in conventional multi-step adhesives
[44,45]. Permeability of simplified total-etch
adhesives was apparent even when wet bonding
was performed with meticulous solvent removal in
vital deep human dentin [41]. This is understand-
able, as the results of the present in vitro study
were generated in the absence of dentin perfusion.
The effects of common errors on sealing ability of total-etch adhesives
Presumably, under in vivo bonding conditions,
additional fluid shifts may occur from patent
dentinal tubules under physiologic pulpal pressures.
Thus, it is speculated that permeability may be
further aggravated when solvent removal is incom-
plete during the course of bonding of total-etch
adhesives to vital deep dentin.
Within the limits of this study, the null hypoth-
esis that there are no differences in dentin bonding
and sealing under the conditions of inadvertent air-
drying and incomplete solvent removal has to be
rejected. Although a collapsed collagen matrix that
results from air-drying of acid-etched dentin
precludes optimal resin infiltration, permeability
is compromised to a lesser extent than bond
strength as there is better resin penetration within
the dentinal tubules to form resin tags. Conversely,
incomplete solvent evaporation may result in
dilution, incomplete polymerization, and phase
separation of resin components. Although both of
these common errors in wet bonding create poorly
infiltrated hybrid layers that are readily susceptible
to long-term bond degradation [25], increased
permeability associated with incomplete solvent
removal may be the most serious bonding error by
creating additional channels for rapid water move-
ment. This, in turn, may enhance water sorption
within the hydrophilic adhesive layers and result in
rapid deterioration of the mechanical properties of
the resin-dentin bonds [45,46]. Several recent
studies demonstrated that longer resin application
times [47] or multiple consecutive coats [48–50]
increased the resin-dentin bond strengths for total-
etch adhesives. The longer diffusion time probably
improved resin infiltration into the exposed col-
lagen matrices. The use of multiple applications of
adhesives also allows more time for removal of
water by inward diffusion of adhesive monomers
and subsequent solvent evaporation from the
interfibrillar spaces. Longer air-drying times for
the uncured adhesives may also help in improving
the evaporation of adhesive solvents and water
derived from dentinal fluids.
Conclusions
Incomplete air-drying of adhesive resins during
bonding results in increased residual water and
other solvents within resin-dentin bonds. This water
may serve as a pathway for additional water
movement. The water permeability of resin-dentin
bonds made without evaporation of solvent, was
greater than that of dry bonding. Longer air-drying
times for the adhesives during wet bonding may
567
help improve the bond strength and reduce
nanoleakage for total-etch adhesives.
Acknowledgements
We graciously acknowledge the technical assistance
provided by Kelli Agee and Amy Wong. The
adhesives examined were generous gifts from
Ivoclar Vivadent and Sybron Kerr. This study was
supported by grants DE 014911 and DE 015306 from
the National Institute of Dental and Craniofacial
Research (PI. David Pashley), and RCG CERG grant
10204604/07840/08004/324/01, Faculty of Dentis-
try, The University of Hong Kong. The authors are
grateful to Michelle Barnes and Zinna Pang for
secretarial support.
References
[1] Frankenberger R, Kramer N, Petschelt A. Technique
sensitivity of dentin bonding: effect of application mistakes
on bond strength and marginal adaptation. Oper Dent 2000;
25:324–30.
[2] Peschke A, Blunck U, Roulet JF. Influence of incorrect
application of a water-based adhesive system on the
marginal adaptation of class v restorations. Am J Dent
2000;13:239–44.
[3] Ferrari M, Tay FR. Technique sensitivity in bonding to vital
acid-etched dentin. Oper Dent 2003;28:3–8.
[4] Nakajima M, Kanemura N, Pereira PN, Tagami J,
Pashley DH. Comparative microtensile bond strength and
SEM analysis of bonding to wet and dry dentin. Am J Dent
2000;13:324–8.
[5] Munksgaard EC. Wet or dry, normal or deproteinized dentin
surfaces as substrate for dentin adhesives. Acta Odontol
Scand 2002;60:60–4.
[6] Barton AFM. Handbook of solubility parameters and other
cohesion parameters. 2nd ed. Boca Raton, FL: CRC Press;
1991 pp. 98–103.
[7] Miller RG, Bowles CQ, Chappelow CC, Eick JD. Application of
solubility parameter theory to dentin-bonding systems and
adhesive strength correlations. J Biomed Mater Res 1998;
41:237–43.
[8] Pashley DH, Carvalho RM, Tay FR, Agee KA, Lee KW.
Solvation of dried dentin matrix by water and other polar
solvents. Am J Dent 2002;15:97–102.
[9] Carvalho RM, Mendonca JS, Santiago SL, Silveira RR,
Garcia FCP, Tay FR, et al. Effects of HEMA/solvent
combinations on bond strength to dentin. J Dent Res
2003;82:597–601.
[10] Eddleston RC, Hindle AR, Agee KA, Carvalho RM, Tay FR,
Rueggeberg FA, et al. Dimensional changes in acid-
demineralized dentin matrices following the use of HEMA-
water versus HEMA-alcohol primers. J Biomed Mater Res
2003;67A:900–7.
[11] Breschi L, Lopes M, Gobbi P, Mazzotti G, Falconi M,
Perdigão J. Dentin proteoglycans: an immunocytochemical
FEISEM study. J Biomed Mater Res 2002;61B:40–6.
568
[12] Suzuki K, Nakai H. Adhesion of restorative resin to tooth
substance—treatment of acid-etched dentin by aqueous
solution. Dent Mater J 1994;12:34–44.
[13] Pashley DH, Zhang Y, Agee KA, Rouse CJ, Carvalho RM,
Russell CM. Permeability of demineralized dentin to HEMA.
Dent Mater 2000;16:7–14.
[14] Nakaoki Y, Nikaido T, Pereira PN, Inokoshi S, Tagami J.
Dimensional changes of demineralized dentin treated with
HEMA primers. Dent Mater 2000;16:441–6.
[15] Pashley DH, Agee KA, Tay FR, Carvalho RM, Terada RSS,
Harmon FJ, et al. Solvent-induced dimensional changes in
EDTA-demineralized dentin matrix. J Biomed Mater Res
2001;56:273–81.
[16] Tay FR, Gwinnett AJ, Pang KM, Wei SH. Variability in
microleakage observed in a total-etch wet-bonding tech-
nique under different handling conditions. J Dent Res 1995;
74:1168–78.
[17] Walshaw PR, McComb D. Clinical considerations for optimal
dentinal bonding. Quintessence Int 1996;27:619–25.
[18] Jacobson T, Söderholm K-J. Some effects of water on dentin
bonding. Dent Mater 1995;11:132–6.
[19] Spencer P, Wang Y. Adhesive phase separation at the dentin
interface under wet bonding conditions. J Biomed Mater
Res 2002;62:447–56.
[20] Reis AF, Oliveira MT, Giannini M, De Goes MF,
Rueggeberg FA. The effect of organic solvents on one-
bottle adhesives’ bond strength to enamel and dentin. Oper
Dent 2003;28:700–6.
[21] Cho BH, Dickens SH. Effects of the acetone content of single
solution dentin bonding agents on the adhesive layer
thickness and the microtensile bond strength. Dent Mater
2004;20:107–15.
[22] Tay FR, Pashley DH. Water treeing—a potential mechanism
for degradation of dentin adhesives. Am J Dent 2003;(16):
6–12.
[23] Li H, Burrow MF, Tyas MJ. The effect of concentration and
pH of silver nitrate solution on nanoleakage. J Adhes Dent
2003;5:19–25.
[24] Chersoni S, Suppa P, Breschi L, Ferrari M, Tay FR, Pashley
DH, et al. Water movement in the hybrid layer after
different dentin treatments. Dent Mater; in press.
[25] Hashimoto M, Ohno H, Sano H, Tay FR, Kaga M, Kudou Y,
et al. Micromorphological changes in resin-dentin bonds
after 1 year of water storage. J Biomed Mater Res 2002;
63B:306–11.
[26] De Munck J, Van Meerbeek B, Yoshida Y, Inoue S, Vargas M,
Suzuki K, et al. Four-year water degradation of total-etch
adhesives bonded to dentin. J Dent Res 2003;82:136–40.
[27] Hashimoto M, Tay FR, Ohno H, Sano H, Kaga M, Yiu C, et al.
SEM and TEM analysis of water degradation of human
dentinal collagen. J Biomed Mater Res 2003;66B:289–98.
[28] Pashley DH, Tay FR, Hashimoto M, Breschi L, Carvalho RM,
Ito S. Degradation of dentin collagen by host-derived
enzymes during aging. J Dent Res 2004;83:216–21.
[29] Pashley DH, Stewart FR, Galloway SE. Effects of air-drying
in vitro on human dentin permeability. Arch Oral Biol 1984;
29:379–83.
[30] Ciucchi B, Bouillaguet S, Holz J, Pashley DH. Dentinal fluid
dynamics in human teeth in vivo. J Endod 1995;21:191–4.
[31] Jacobsen T. Bonding of resin to dentin. Interactions
between materials, substrate and operators. Swed Dent
J Suppl 2003;160:1–66.
M. Hashimoto et al.
[32] Bouillaguet S, Duroux B, Ciucchi B, Sano H. Ability of
adhesive systems to seal dentin surfaces: an in vitro study.
J Adhes Dent 2000;2:201–8.
[33] Gregoire G, Joniot S, Guignes P, Millas A. Dentin
permeability: self-etching and one-bottle dentin bonding
systems. J Prosthet Dent 2003;90:42–9.
[34] Momoi Y, Akimoto N, Kida K, Yip KH, Kohno A. Sealing ability
of dentin coating using adhesive resin systems. Am J Dent
2003;16:105–11.
[35] Özok AR, Wu M-K, De Gee AJ, Wesselink PR. Effect of dentin
perfusion on the sealing ability and microtensile bond
strengths of a total-etch versus an all-in-one adhesive. Dent
Mater 2004;20:479–86.
[36] Vaidyanathan J, Chinnaswamy K, Vaidyanathan TK. Biomi-
metic recognition and immunochemical assay of ligand
binding to collagen. J Adhes Dent 2003;5:7–17.
[37] Tay FR, Gwinnett AJ, Wei SHY. Relation between water
content in acetone/alcohol based primer and interfacial
ultrastructure. J Dent 1998;26:147–56.
[38] Tay FR, Gwinnett AJ, Wei SHY. Micromorphological
spectrum from overdrying to overwetting acid-conditioned
dentin in water-free, acetone-based, single-bottle primer/-
adhesives. Dent Mater 1996;12:236–44.
[39] Tay FR, Pashley DH, Suh BI, Carvalho RM, Itthagarun A.
Single-step adhesives are permeable membranes. J Dent
2002;30:371–82.
[40] Chersoni S, Suppa P, Grandini S, Goracci C, Monticelli F,
Yiu C, et al. In vivo and in vitro permeability of one-step
self-etch adhesives. J Dent Res 2004;83:459–64.
[41] Tay FR, Frankenberger R, Krejci I, Bouillaguet S, Pashley
DH, Carcalho RM, et al. Single-bottle adhesives behave as
permeable membranes after polymerization. I. In vivo
evidence. J Dent (in press).
[42] Hashimoto M, Ito S, Tay FR, Svizero NR, Sano H, Kaga M,
et al. Fluid movement across the resin-dentin interface
during and after bonding. J Dent Res 2004;11:843–8.
[43] Hashimoto M, Tay FR, Ito S, Sano H, Kaga M, Pashley DH.
Permeability of adhesive resin films. J Biomed Mater Res; in
press.
[44] Tay FR, Pashley DH. Dentin adhesives: have they become
too hydrophilic? J Can Dent Assoc 2003;69:724–31.
[45] Tay FR, Hashimoto M, Pashley DH, Peters MC, Lai SC, Yiu CK,
et al. Aging affects two modes of nanoleakage expression in
bonded dentin. J Dent Res 2003;82:537–41.
[46] Yiu CKY, King NM, Pashley DH, Suh BI, Carvalho RM,
Carrilho MRO, et al. Effect of resin hydrophilicity and
water storage on resin strength. Biomaterials 2004;25:
5789–96.
[47] Asakawa T, Manabe A, Itoh K, Tani C, Inoue M, Sasa R. Effect
of multiple application of dentin bonding agent on marginal
integrity of resin composite. J Clin Pediatr Dent 2002;26:
257–61.
[48] el-Din AK, Abdel-Mohsen MM. Effect of changing application
times on adhesive system bond strengths. Am J Dent 2002;
15:321–4.
[49] Hashimoto M, De Munck J, Ito S, Sano H, Kaga M, Oguchi H,
et al. In vitro effect of nanoleakage expression on resin-
dentin bond strengths analyzed by microtensile bond test,
SEM/EDX and TEM. Biomaterials 2004;25:5565–74.
[50] Hashimoto M, Sano H, Yoshida E, Hori M, Kaga M, Oguchi H,
et al. Effects of multiple coatings on dentin bonding. Oper
Dent 2004;29:416–23.