Journal of Dentistry (2005) 33, 549559

www.intl.elsevierhealth.com/journals/jden

Effect of smear layer thickness and acidity of

self-etching solutions on early and long-term
bond strength to dentin
Alessandra Reisa,*, Viviane Grandia, Larissa Carlottoa, Giana Bortolia,
Rafael Patzlaffa, Maria de Lourdes Rodrigues Accorinteb,
Alessandro Dourado Loguercioa
a

Department of Dental Materials and Operative Dentistry, Universidade do Oeste de Santa Catarina,
lio Vargas, 2125, Bairro Flor da Serra, CEP: 89600-000 Joacaba/SC, Brazil
Campus Joacaba, R. Getu
b
o Paulo, Sa
o Paulo, SP, Brazil
Department of Dental Materials, Universidade de Sa
Received 12 May 2004; received in revised form 18 October 2004; accepted 10 December 2004

KEYWORDS
Self-etching
adhesives;
Total-etch adhesives;
Smear layer thickness;
Microtensile test;
Ultimate microtensile
strength;
Long-term
bond
strength;
Resindentin
bond
strength;
Dentin adhesion

Summary Objectives. To evaluate the effect of smear layer thickness (SL) on early
and 6-month bond strength (BS) of self-etching adhesives to dentin and to measure
the ultimate microtensile strength (UTS) of the adhesives.
Methods. Clearfil SE Bond; Optibond Solo Plus Self-Etch Primer; Tyrian Self Priming
Etchant (TY) and as controls, Single Bond (SB) and Scotchbond Multi-Purpose Plus
(SBMP) were applied on flat superficial dentin surface with thick and thin SL
thicknesses. After adhesives application (nZ6) a resin build-up was made. After
24 h, resindentin beams (0.8 mm2) were prepared to be tested immediately and after
6-month (6M) at 0.5 mm/min. For the UTS measurement, hour-glass specimens were
prepared with the bonding resin alone or after mixing (1:1). BS values were analyzed by
three-way repeated measures ANOVA and Tukeys multiple comparison tests.
Two-way ANOVA (bonding resin and bonding resinCself-etching primer) and Tukeys
test were used for the UTS values. The bonding resins were re-evaluated separately by a
one-way ANOVA and Tukeys test, since Single Bond is a one-bottle adhesive (aZ0.05).
Results. The SL thickness was not significant (pZ0.64). BS values were reduced
after 6M, except for the SBMP. TY provided the lowest BS mean while SB and SBMP the
highest BS. The UTS of the SBMP was the highest. TY yielded the lowest UTS.
Regression analysis revealed a linear and significant relationship between the UTS of
self-etch systems and the mean BS (RZ0.95, pZ0.02).
Conclusions. The performance of a self-etching system does not seem to be
dependent on the SL thickness. The total-etch, three-step system provided the
highest BS to dentin and maintained the BS stable over 6 months. The performance of
the self-etching systems can be envisaged by their UTS.
q 2005 Elsevier Ltd. All rights reserved.

* Corresponding author. Tel./fax: C55 49 551 2004.

E-mail address: reis_ale@hotmail.com (A. Reis).
0300-5712/$ - see front matter q 2005 Elsevier Ltd. All rights reserved.
doi:10.1016/j.jdent.2004.12.003

550

Introduction
Total-etch systems require a conditioning, a rinsing
and a priming step in order to allow encapsulation
of collagen fibers by the resin monomers and the
formation of the so-called hybrid layer.1 Demineralization of intertubular dentin and maintenance of interfibrillar porosity is required for
monomer penetration into dentin. Thus, wet bonding technique has been designated as essential for
the current adhesive systems in order to prevent
the known collapse of collagen fibrils in air-dried
conditions.2,3 The proper degree of moisture is
individual for each solvent-based adhesive system;4,5 however, even under ideal condition, an
actual discrepancy between the extent of the
demineralization and monomers infiltration is likely
to occur.68 The development of self-etch systems
avoided the occurrence of the above disadvantages
from total-etch systems. This bonding approach has
reintroduced the concept of employing the smear
layer as a bonding substrate, but with novel insights
and improved formulas that can etch beyond the
smear layer into the underlying dentin. Simultaneous infiltration of the demineralized dentin
matrix during acid etching is possible, as the
demineralizing component of the primer is also
the infiltrating resin.9
The hybridized complex of self-etch systems is
comprised of a surface zone of hybridized smear
layer and a subsurface zone of hybridized intertubular dentin.1012 To achieve this goal, the selfetching primer should penetrate beyond the smear
layer into the intact, mineralized dentin. Under
clinical circumstances, the thickness, coarseness,
and roughness of smear layers may vary according
to the rotary instruments used for cavity preparation.13,14 Thick smear layers might affect the
ability of self-etching systems to penetrate through
intact, mineralized dentin, since early neutralization of the adhesive by the dentin buffering
components presented in the smear layer15 might
hamper superficial demineralization of solid dentin,
which is required for collagen exposure. Studies
addressing this matter have not reached a conclusion about the performance of self-etching
systems applied to varied smear layer thickness.
Some studies reported low resindentin bond
strengths over thick dentin smear layers,1618
while others reported no influence of smear layer
thickness on resindentin bond strengths.11,13
To the authors knowledge, there is no information as to whether the thicknesses of smear
layers incorporated in the hybridized complex
affect the long-term resindentin bond strength.

A. Reis et al.
Other important issue that has been disregarded in
most studies and may play a role on the adhesive
performance is the ultimate strength of the
adhesive systems employed. Therefore, the objective of this study was to determine the effects of
varied dentin smear layer thicknesses on the early
and six-month bond strength of three two-step selfetching systems possessing different levels of
acidity, and to measure the ultimate microtensile
strength of the bonding resin and the self-etching
primer. The null hypothesis to be tested was:
(1) there will be no influence of smear layer
thicknesses on early and 6-month bond strengths
to dentin; (2) the bond strengths over thick and thin
smear layer covered dentin will not be dependent
on the acidity of self-etch systems and; (3) the
ultimate strength of the adhesives will not be
different among each other.

Materials and methods

Experimental design and teeth preparation
This study had the approval of the Ethical Committee of the University of Sa
o Paulo, School of
Dentistry. Thirty non-carious, human third molars
were used. The teeth were disinfected in 0.5%
chloramine and used within 6 months following
extraction. The occlusal enamel was wet ground
using a 180-grit SiC paper, in order to expose a
superficial flat dentin surface. The teeth were
longitudinally sectioned in a buccal to lingual
direction (Labcut 1010, Extec Corp., Enfield, CT,
USA) into two halves (Fig. 1). The occlusal surface
of one half was further polished with wet 600-grit
SiC paper for 60 s to create thin smear layer and the
other half was treated alike with a 60-grit SiC (thick
smear layer). Then, six teeth were randomly
assigned into five experimental groups (Fig. 1).
Three self-etching adhesive systems were
selected according to their acidity, as provided by
the manufacturers: Clearfil SE Bond (SEKuraray
Medical, Inc., Osaka, Japan)mild (pHO2), Optibond Solo Plus Self-Etch PrimerCOptibond
Solo Plus (SOKerr; Orange, CA, USA)moderate
(1!pH!2) and Tyrian Self Priming Etchant (SPE)C
One-Step Plus (TYBisco, Schaumburg, IL, USA)
aggressive (pH!1). Other two total-etch adhesive
systems were used as controls: Single Bond (SB3M
ESPE, St Paul, MN, USA), a two-step adhesive
system, and Scotchbond Multi Purpose Plus
(SBMP3M ESPE), a three-step adhesive system.
Their composition, application mode, and batch
number are described in Table 1.

Long-term bond strength of the self-etching primers to dentin

Figure 1

551

Experimental design.

Restorative procedure
A single operator applied on superficial dentin all
the adhesive systems, according to Table 1. The
bonding procedure was performed under controlled
temperature and humidity (24 8C and 50% relative
humidity). Special care was taken to ensure that the
dentin surfaces were adequately covered by monomers after evaporation of the solvents. In the event
that matte dentin was encountered, additional
coats of adhesives were applied to produce shiny
surfaces prior to light-activation of the adhesives. A
VIP light-curing unit with a light intensity of
600 mW/cm2 (Bisco, Schaumburg, IL, USA) was
used throughout the restorative procedure. Following the adhesive application, resin composite buildups (Z 250, 3M ESPE, St Paul, MN, USA) were
constructed in 1 mm increments, and light-cured
for 30 s each.

Specimen preparation and microtensile bond

strength
After a 24-h storage in distilled water at 37 8C, the
specimens were longitudinally sectioned in both xand y-directions across the bonded interface with a
water-cooled diamond saw in a Labcut 1010
machine (Extec Corp., Enfield, CT, USA), to obtain
bonded sticks per hemi-tooth, each with a crosssectioned area of approximately 0.8 mm2. The
bonded sticks originated from the same teeth
were randomly divided and assigned to be tested
immediately or after 6 months of storage in
distilled water containing 0.4% sodium azide at

37 8C. The storage solution was not changed19 and

its pH was monitored monthly.
The number of premature debonded sticks (D)
per hemi-tooth during specimen preparation was
recorded. Specimens originated from the areas
immediately above the pulp chamber had their
remaining dentin thickness (RDT) measured with a
digital caliper and recorded (Absolute Digimatic,
Mitutoyo, Tokyo, Japan). The cross-sectional area
of each stick was measured with the digital caliper
to the nearest 0.01 mm and recorded for the bond
strength (BS) calculation.
At each storage time period, individual bonded
sticks were attached to the Geraldelis device for
microtensile testing with cyanoacrylate resin
(Zapit, Dental Ventures of North America, Corona,
CA, USA) and subjected to a tensile force in a
universal testing machine (Emic, Sa
o Jose
dos
Pinhais, PR, Brazil) at a crosshead speed of
0.5 mm/min. The bond failure modes were evaluated at X400 (HMV-2, Shimadzu, Tokyo, Japan) and
classified as (1) cohesive within dentin; (2) cohesive
within composite resin and (3) adhesive/mixed
(failure at resin/dentin interface or mixed with
cohesive failure of the neighboring substrates).

Specimen preparation and ultimate

microtensile strength
The bonding resin either mixed or not with the selfetching primer (1:1) was dropped in a compound
impression mold 10 mm long, 2 mm wide and 1 mm
deep, and gently air-dried oil and water-free
compressed air (20 s) to allow for solvent

552

Table 1

Adhesive systems and application mode.

Adhesive systems

Composition

Application mode

Batch number

Clearfil SE BondSE
(Kuraray)

1. Primerwater, MDP, HEMA, camphoroquinone, hydrophilic dimethacrylate

2. AdhesiveMDP, Bis-GMA, HEMA, camphoroquinone,
hydrophobic dimethacrylate, N,N-diethanol p-toluidine
bond, silanated colloidal silica

1- Application of two coats of the primer with

slight agitation (20 s)
2- Air-dry (10 s at 20 cm)

00176A001185A

3- Application of one coat of the adhesive (15 s)

4- Air -dry (10 s at 20 cm)
5- Light activation (10600 mW/cm2)
Optibond Solo Self-EtchPrimer and Optibond
Solo PlusSO (Kerr)

1. Alkyl dimethacrylate resins, Barium aluminoborosilicate glass, fumed silica (silicon dioxide), sodium hexafluorosilicate and ethyl alcohol
2. Alkyl dimethacrylate resins (2528%), ethyl alcohol,
water, stabilizers and activators

1- Application of one coat of the primer with slight

agitation (15 s)

205187203D20

2- Air-dry for 10 s at a distance of 20 cm

3- Application of 1 coat of the adhesive (15 s with
slight agitation)
4- Air-dry (10 s at 20 cm)
5- Application of 1 coat of the adhesive (15 s with
slight agitation)
5- Air-dry (10 s at 20 cm)
6- Light-activation (20 s600 mW/cm2)

Tyrian SPE and One Step

PlusTY (Bisco)

1. Self-etching2-acrylamido-2-methyl propanesulfonic
acid (215%); Bis-GMA; Ethanol (2550%)
2. Adhesive-Bis-GMA, BPDM, HEMA, Glass Frit initiator and
acetone (4070%)

1- Mixture of Tyrian SPE (A and B) and application

of 2 coats with slight agitation (10 s)
2- Air-dry (10 s 20 cm)

200002694
200004295

3- Application of 2 consecutive coats of the

adhesive, brushing for 10 s each
4- Air-dry (10 s 20 cm)
5- Light-activation (10 s600 mW/cm2)
Single BondSB (3M
ESPE)

1. 37% phosphoric acid

2. AdhesiveBis-GMA, HEMA, dimethacrylates, polyalknoic
acid copolymer, initiators, water and ethanol

2GM

A. Reis et al.

1- Acid etching (15 s), rinsing (15 s) and air-drying

(10 s) leaving dentin moist
3- Application of one coat of the adhesive (10 s
with slight agitation)
4- Air-dry (10 s at 20 cm)
5- Application of 1 coat of the adhesive (10 s with
slight agitation)
6- Air-dry (10 s at 20 cm)
7- Light-activation (10 s600 mW/cm2)

2. Primeraqueous solution of HEMA, polyalkenoic acid

copolymer (Vitrebond)
3. AdhesiveBis-GMA, HEMA, dimethacrylates and
initiators

ScotchBond Multi Purpose PlusSBMP (3M

ESPE)

1. 37% phosphoric acid

5- Application of 1 coat of the adhesive (10 s with

slight agitation)
6- Air-dry (10 s at 20 cm)
7- Light-activation (10 s600 mW/cm2)

1- Acid etching (15 s), rinsing (15 s) and air-drying

(10 s) leaving dentin moist
3- Application of 2 coats of the primer (10 s with
slight agitation)
4- Air-dry (10 s at 20 cm)

30087543

Long-term bond strength of the self-etching primers to dentin

553

evaporation. Then, a plastic matrix strip was placed

on the adhesive and the surface was light-cured for
20 s at 600 mW/cm2. This protocol, however, was
not enough to permit the One Step Plus associated
or not with Tyrian SPE to polymerize. Thus, for this
adhesive system, an air-stream of 120 s followed by
light-curing for 120 s was needed to assure polymerization of the specimens. Using shorter periods of
time for solvent evaporation and light-curing, the
specimens got a rubbery and sticky appearance.
Five specimens were performed for each experimental condition. After a 24-h storage in distilled
water at 37 8C, the specimens were hand-free
trimmed with a fine diamond bur, under water
cooling, to an hour-glass shape with a crosssectional area of approximately 0.8 mm2. Then,
the ultimate microtensile strength (UTS) was
measured as previously described for resindentin
beams.

Statistical analysis
A bond strength index (BS) was calculated for each
hemi-tooth used per group as described by Reis
et al.5 The BS index is a weighted mean assuming
the relative contribution of the possible mode of
failures. The cohesive strength of the resin composite and the cohesive strength of dentin are
considered as the average value of all the specimens (from a single tooth) that failed in that
manner. The prematurely debonded specimens
were included in the BS index. The average value
attributed to specimens that failed prematurely
during preparation is arbitrary, and corresponds to
approximately half of the minimum bond strength
value that could be measured in this study
(ca. 10.4 MPa).
The microtensile BS indexes were subjected to
a three-way repeated measures analysis of variance and a post hoc test (Tukeys test at
aZ0.05) for pair-wise comparisons. The period
of evaluation (immediate or 6 months) was the
repeated factor. An additional random factor was
added to the statistical model as correction for
the two samples (hemi-tooth) gathered from the
same tooth.20
The UTS of the adhesive systems was subjected
to a two-way analysis of variance (factors: bonding
resin and bonding resinCself-etching primer).
Tukeys test was used for pair-wise comparisons
(aZ0.05) among averages. As Single Bond is a onebottle adhesive, the ultimate strength of the
bonding resins were evaluated separately by a
one-way ANOVA (aZ0.05) and Tukeys test for
pair-wise comparisons (aZ0.05).

554

A. Reis et al.

Table 2 Percentage of specimens (%) according to the fracture patterna or premature debonding (D) for each
experimental condition.
Adhesive systems

Time
Immediate

Fracture pattern

A/M

Clearfil SE Bond
Optibond Solo Self-Etch PrimerC
Optibond Solo Plus
Tyrian SPECOne Step Plus
Scotchbond Multi Purpose Plus
Single-Bond

85.3
87.1

11
9.2

0
0

86
89.7
89.9

0
7.7
7.2

0
0
0

6 months
PD

A/M

PD

3.7
3.7

73.7
56.3

4.3
7.8

4.4
15.1

17.6
20.8

14
2.6
2.5

72.6
74
94.5

0
7.1
0

1.6
7.7
0

25.8
11.2
5.5

Data are expressed in percentage values.

a
A/M, adhesive or mixed failure; C, cohesive failure in dentin; R, cohesive failure in resin; PD, premature debonded sticks.

The correlation between the UTS of the selfetching primers and their mean BS were
analyzed by simple linear regression analysis.
The strength of the association between these
two variables (UTS vs. BS) was estimated with the
Pearson productmoment correlation statistics
(aZ0.05).

Results
The mean cross-sectional area ranged from 0.78 to
0.89 mm2 and no difference among the treatment
groups was detected (pO0.05).
The average strength of all specimens that failed
cohesively in dentin was 38.5 MPa (38.5G9.1,
nZ16). The average strength of all specimens
that failed cohesively in resin was 50.0 MPa
(50.0G8.3, nZ13). The percentage of sticks that
had a premature failure during specimen preparation as well as the frequency of each fracture
pattern in each group is shown in Table 2. The
means and standard deviations of the BS indexes are
shown in Table 3.
Three-way repeated measures ANOVA did not
detect statistical significant effects for the

interactions (p!0.05). The main categorical variable smear layer thickness was not statistically
significant (pZ0.64). A significant effect of
the storage time on bond strengths was detected
(pZ0.0001). Reductions in BS were observed after
the 6-month storage, except for the SBMP (Table 3).
Regarding the main categorical factor adhesive,
significant differences were detected (pZ0.001).
The lowest BS mean was observed for Tyrian SPEC
One Step Plus which was statistically different from
all the others (Table 3). The highest BS was found
for the SBMP.
The means and standard deviations of the UTS
are shown in Table 4. As detected by two-way
ANOVA, the UTS of the bonding resins whether
associated or not with their self-etching primer
were different (pZ0.001). The highest UTS of the
bonding resin were found for the SBMP, while the
lowest was One Step Plus and Single Bond. Similar
trends were observed when the bonding resin was
mixed with the primer solution, i.e. the SBMP
adhesive had the best performance while Tyrian
SPECOne Step Plus had the worst. For the same
adhesive system, there was a trend towards a
reduction in the UTS when the bonding resin was
mixed with self-etch primer. However, this

Table 3 Means, standard deviations (MPa) and statistical significance of bond strength indexes at each
experimental condition.
Adhesive systems
Clearfil SE bond
Optibond Solo Self-Etch PrimerC
Optibond Solo Plus
Tyrian SPECOne Step Plus
Scotchbond Multi Purpose Plus
Single-Bond

Time
Immediate

6 months

40.6G4.7 (53) a
36.2G4.0 (55) a,b

26.6G4.1(42) b,c
24.6G2.4(41) b,c

24.1G3.7(42) b,c
42.6G5.5(66) a
41.5G2.6(72) a

18.6G2.8(28) c
45.2G4.3(60) a
28.0G2.6(65) b,c

Same symbols indicate similar means (pO0.05). Values in parentheses are the number of specimens tested.

Long-term bond strength of the self-etching primers to dentin

555

Table 4 Means, standard deviations (MPa) and statistical significance of the ultimate bond strength for each
adhesive system.
Bonding resin

(*)

(**)

Bonding resinC
primer

(*)

Scotchbond Multi
Purpose Plus
Adhesive
Clearfil SE Bond
Optibond Solo Plus
Adhesive
One Step Plus

38.4G4.2 a

Scotchbond Multi
Purpose Plus

32.9G2.3 a,b

26.5G3.7 b
15.5G3.3 c,d

b
m

Clearfil SE Bond
Optibond Solo

27.3G2.6 b
12.7G2.1 d

m, f

Tyrian SPECOne
Step Plus

5.1G0.8 e

Single-Bond

8.7G0.9 d
10.1G1.2

(*) Comparison between the bonding resins and the bonding resins plus primer, excluding Single-Bond. Means with the same letters
are statistically similar (pO0.05). (**) Comparison between the bonding resins. Means with the same symbols are statistically similar
(p!0.05).

difference was only significant for the adhesive

One-Step Plus (pZ0.01).
Regression analysis revealed a linear and positive
significant relationship between the UTS of the
self-etching systems and the mean BS index (Fig. 2)
(RZ0.95, pZ0.02). When we attempted to include
the total-etch systems in the regression analysis, a
linear relationship was also observed, however,
no statistical significance was detected (RZ0.78,
pZ0.24).

Discussion
In the last decade, bonding to smear-covered
dentin was not successful because early

Figure 2 Correlation and linear relationship between

the mean ultimate strength values (MPa) and the mean
resindentin bond strengths (MPa) (OSCTYZOne Step
PlusCTyrian SPE; OBCSEZOptibond Solo PlusCOptibond Solo Self-etch Primer; CSCCPZClearfil SE BondC
Clearfil SE Primer).

formulations of self-etch systems did not contain

enough acidic monomers to penetrate through the
smear layer into the mineralized dentin substrate.
This fact lead clinicians to abandon the self-etch
approach and employ adhesive systems based on
the total-etch concept. Concerns about the smear
layer thicknesses were left apart because the
3040% phosphoric acid, usually used as conditioner, is acidic enough to remove completely the
smear layer and smear plugs and also promote a
demineralization of the underlying mineralized
dentin, exposing collagen fibrils, which are thereafter infiltrated by monomers.21
Contemporary self-etch systems have been
developed by increasing the concentration of acidic
resin monomers and combining them with HEMA.22
Then an increased interest on the study of the
interaction between these systems and smear layer
thicknesses occurred. A great variety of self-etch
systems are presented in the market. They differ in
the number of bottles, steps, and acidity of the
primer solution. It might be speculated that selfetch systems with higher pH are less effective in
solubilizing thick smear layers and demineralizing
solid dentin surface for hybridization than
adhesives with lower pH. Although this is still a
controversial matter, some authors have reported
reduced bond strength values for some self-etch
systems when applied over thick smear layer.1618
On the other hand, Tay et al.11 reported that the
microtensile bond strength of Clearfil SE Bond, a
mild self-etching adhesive, was not affected by
various thicknesses of the smear layers created by
#60-, #180-, or #600-grit abrasive papers or the
absence of smear layer. Similarly, Tani and Finger13
reported that the shear bond strengths of the three
all-in-one self-etch adhesives were not affected by

556
the dentin surface condition. The results of the
present investigation agree with these studies,
demonstrating that the smear layer thickness has
no influence on the early bond strength values.
Thus, the first null hypothesis was accepted.
These observations suggest that either the
buffering capacity of the smear layer is weak, or
the smear layer does not prevent the primer from
penetrating into the underlying mineralized dentin
matrix.11,12 The smear layer is, in fact, a disaggregated substrate full of easily penetrable subunits with interconnecting channels. 23 This
morphology enhances diffusion and allows acidic
monomers to reach the basal portion of the smear
layer easily, irrespective of their aggressiveness
potential. As the smear layer is a very porous
substrate, the acidic monomers diffuse freely until
they reach the mineralized substrate underneath.
This is somewhat true, that Tay et al.11,12 demonstrated that the authentic hybrid layer thickness
produced by a mild self-etch system did not vary
even in the absence or presence of varied smear
layer thicknesses.
Irrespective of the smear layer thickness, the
self-etching systems showed different bond
strength performances and thus the second null
hypothesis was rejected. As already demonstrated
by other authors, it seems that the depth of
penetration of self-etch adhesives into subsurface
dentin varies according to the acidity of the selfetch system.24 Thin authentic hybrid layers are
formed with a mild self-etch adhesive, as Clearfil SE
Bond (approximately 0.5 mm thick) whereas a
moderate and an aggressive self-etch system
usually forms thicker hybrid layers, in the range of
1.22.2 and 2.55.0 mm, respectively.
Conversely, a close analysis of bond strengths of
self-etch systems with different levels of acidity
indicates that the aggressive ones, as Tyrian SPE
(Table 3), usually present low bond strength
values.2527 In fact, previous literature reports
have demonstrated that there is no correlation
between bond strengths and hybrid layer thickness,28,29 and thus it seems that the ability to
create thick hybrid layers cannot be considered as
an additional advantage for improved retention.
These observations suggest that other factors are
involved in the performance of a self-etch system.
For instance, Pashley et al.30 showed, using a
modeling approach, that the theoretical strength
of the resindentin bond strength should be proportional to the strength of the adhesive used to
infiltrate demineralized dentin. The present study
has found a strong correlation between the resin
dentin bond strengths and the mechanical
properties of cured resin for the self-etch systems,

A. Reis et al.
and thus the third null hypothesis was rejected.
This finding is in agreement with other laboratory
investigation,31 and they confirm the observations
of the theoretical modeling approach. This means
that by knowing the ultimate strength of a self-etch
system, one may envisage their bonding
performance.
Another important aspect is the amount of the
solvents included in the self-priming solution.
Water is present in all the self-etch systems
employed because it is an essential component to
enable ionization of the acidic monomers and
demineralization of dental hard tissues. As Tyrian
SPE is very acidic, it is likely that its solvent content
may be higher than the others self-etch systems, in
order to promote complete ionization of the acidic
monomers. Consequently, the thickness of the
adhesive layer, after solvent evaporation, can be
very thin and an incomplete polymerization due to
oxygen inhibition may occur.32,33 This partially
explains why aggressive self-etch primers demonstrated higher resindentin bond strengths when
several coats of the primer were applied.33 The
lower the remaining solvent content, the higher the
mechanical properties of the polymer formed,
which is a relevant property for the integrity of
adhesive interfaces.34,35 This seems to be particularly important for some adhesive systems. For
instance, it was not possible to obtain One-Step
specimens without increasing the air-stream period
to allow solvent evaporation and increasing the
light-curing time. Even under improved conditions
the ultimate strength of One-Step systems was
lower than for the other systems (Table 4). The high
amount of solvents in its composition (unpublished
data) may prevent the attainment of an adequate
degree of conversion, which is in turn responsible
for the low mechanical properties of this system
and possibly of the low resindentin bond
strengths.35 This situation got even worse when
the bonding resin One-Step was mixed with the selfpriming Tyrian SPE, which was probably due to an
increase in the amount of solvent within the mass of
the bonding resin. Besides that, the addition of
acidic monomers to polymerisable resins causes
reduction of their ultimate tensile strength. In a
clinical situation, it is possible that the application
of acidic primers or adhesives to dentin will render
acidity buffered, and may improve the degree of
conversion of the polymer after contact with
dentin. By preparing the specimens in a compound
mold, while solvents may evaporate, the acidic
monomers are not buffered, and that may compromise their polymerization.
Recently, Carrilho et al.36 have reported the
ultimate microtensile strength of some adhesives

Long-term bond strength of the self-etching primers to dentin

tested (OS and SB) in this study and they found
values somewhat higher than the ones obtained.
This could be attributed to differences in the
specimen preparation, time allowed for solvent
evaporation and the exposure time for curing. In
the present investigation, we attempted to use an
exposure time equivalent to those used in a clinical
setting, while in the Carrilhos study, the specimens
were over cured.
The results of the present investigation demonstrated reductions on the bond strength values after
a 6-month water storage for all adhesive systems,
irrespective of the smear layer thickness (see
Table 3), leading us to reject the third null
hypothesis. As the smear layer is a porous substrate,
the expectation was that thick smear layers could
work as water reservoir and accelerate the degradation of the bonds. However, this expectation was
not confirmed in the present study. It is likely that
the hybridized smear layer has as much affinity with
water as does the authentic hybrid layer. The lack
of correlation between the bond strengths of selfetching systems and the smear layer thickness can
be considered as an advantage, since it is clear from
the literature findings that the thickness of the
smear layer can vary according to the rotary
instrument selected,13,18 and this selection is not
based on the clinicians like but on the aim of the
restorative procedure.
The degradation of resindentin bonds was firstly
attributed to hydrolysis of collagen fibrils at the
base of the hybrid layer due to the incomplete
penetration of resin monomers.37,38 In fact, discrepancies between the extent of demineralization
and resin infiltration may not be the sole reason for
bond strength decrease. Although this would
explain the reductions observed for the total-etch
two-step Single Bond, this would not explain the
results with the self-etch adhesives, which also
showed degradation of the resindentin bonds over
the 6-month water storage in the present investigation as well as in others.39,40
Therefore, other factors should be considered.
Hydrolytic degradation of polymers observed after
water sorption and the permeability of the adhesive
layer are likely the cause. Polymer systems present
several nanometer-sized pores which are crucial in
establishing the equilibrium moisture uptake. They
are located at the cross-link junctions, which are
also the locations of the polar hydroxyls and
amines. The volume fraction of these nanopores
) is a function of temperature.41 How(5.06.0 A
ever, polarity is of primary importance: highly polar
resins absorb more water than less polar ones.41
Hydrophilic resins, such as those present in the
current adhesives, are highly prone to absorb

557

water.42 Since all adhesives used in the present

study contain significant amounts of hydrophilic
monomers, water sorption over time can also be
regarded as a contributor to the observed reduction
in bond strengths. The water sorption reduces the
intermolecular interactions between the polymer
chains, reducing the mechanical properties of the
polymer.43 Besides that, it is well documented from
in vitro and in vivo studies that simplified adhesives
may behave as semipermeable membranes after
polymerization.4446 The lack of an additional coat
of a hydrophobic bonding resin and the presence of
hydrophilic groups in the self-etch adhesive monomers continue to draw water from the underlying
hydrated dentin47 and from the oral environment48
after polymerization.
The exception is the total-etch, three-step
adhesive system Scotchbond Multi-Purpose Plus.
This system has a primer solution, composed
basically from solvents and hydrophilic monomers,
and a bonding resin composed of hydrophobic resins
which are applied over the hydrophilic primer. The
ultimate strength of this adhesive system is a good
predictor of its superiority among the others. The
complete absence of solvents in the bonding resin
allows the formation of a high cross-linked polymer
with a high degree of conversion. After mixing the
bonding resin with the primer, the ultimate
strength of this system was not significantly
reduced, probably due to the low amount of solvent
per total mass of the bonding resin. It is likely that
the lower affinity with water presented by this layer
(highly cross-linked polymer with predominance of
hydrophobic monomers) has minimized water sorption and thus enabled stability of resindentin bond
strengths over time (Table 3). This finding is in
agreement with the study of De Munck et al.20 The
authors demonstrated that two total-etch, threestep systems, including the one evaluated in this
study, showed no reduction on bond strength values
after a 4-year water storage. In contrast, other two
total-etch, two-step system showed remarkable
reductions on resindentin bond strengths. The
formation of a separate coupling resin layer,
which is more hydrophobic as compared to the
two-step systems may have resulted in the low
sensitivity to water degradation. This means that
the weak link within the hybrid layer, over time, is
probably the high polarity of the hydrophilic
monomers used in the adhesive systems.36,41,43
Although the results of the present investigation
and others 21 apparently indicate that more
hydrophobic adhesive systems seems to be more
resistant to water degradation, there has been
authors that did not report coinciding findings.28
This apparent controversy and lack of studies

558
evaluating total-etch, three-step adhesives over
time encourage future studies on this matter.

Acknowledgements
The authors are grateful to the Dental School of
UNOESC, Joac
aba (SC). This study was partially
supported by CAPES and CNPq Grants
(551049/2002-2; 350085/2003-0; 302552/2003-0
and 474225-2003-8).

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