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Ethanol-wet Bonding Technique May Enhance

the Bonding Performance of Contemporary
Etch-and-Rinse Dental Adhesives

Article in The journal of adhesive dentistry June 2011

DOI: 10.3290/j.jad.a21853 Source: PubMed

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Ethanol-wet Bonding Technique May Enhance the te n
ot

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fo r

Bonding Performance of Contemporary Etch-and-Rinse

Dental Adhesives
Fang Lia / Xiao-Yang Liub / Ling Zhangc / Jun-Jun Kangd / Ji-Hua Chene

Purpose: To determine whether bonds of contemporary etch-and-rinse adhesives made with ethanol-wet bonding
are stronger and more durable than those made with water-wet bonding, and to explore the possible reasons for
the bonding results.
Materials and Methods: Flat surfaces of midcoronal dentin were made in extracted human third molars. The
dentin surfaces were randomized into 6 groups according to bonding techniques (water- vs ethanol-wet bonding)
and dental adhesives [Single Bond 2 (SB), Prime Bond NT (PB), and Gluma Comfort Bond (GB)]. After etching
and rinsing, dentin surfaces were either left water-moist or immersed in ethanol. Following adhesive application
and composite buildups, the bonded teeth were sectioned into beams for microtensile bond strength evaluation
with or without NaOCl challenge. The morphology of the hybrid layer was analyzed with SEM. The wettability of
water- vs. ethanol-saturated dentin was evaluated. The concentrations of non-volatile ingredients in the adhe-
sives were compared.
Results: Compared to water-wet bonding, ethanol-wet bonding yielded similar (p > 0.05 for PB and GB) or higher
(p < 0.05 for SB) 24-h bond strength, displayed significantly higher bond strength after chemical challenge (p <
0.05, for all three adhesives), and produced more even hybrid layers. Moreover, ethanol-saturated dentin exhib-
ited a lower contact angle than water-saturated specimens, and the concentrations of non-volatile ingredients of
the adhesives decreased in the order of SB > GB > PB.
Conclusion: Ethanol-wet bonding could improve the bonding efficacy of contemporary etch-and-rinse adhesives,
probably due to the good wettability of ethanol-saturated dentin and the structure of the hybrid layer. Moreover,
this positive effect of ethanol-wet bonding might be influenced by the composition of adhesives.

Keywords: dentin bonding, ethanol-saturated dentin, hybrid layer, wettability.

J Adhes Dent 2011;13:xxpages Submitted for publication: 29.11.10; accepted for publication: 16.02.11

a Dentist, Department of Prosthodontics, School of Stomatology, Fourth

Military Medical University, Xian, China. Experimental design, wrote manu-
script.
b Researcher, Department of Quality Validation, Xian Janssen Pharmaceutical
Ltd. Xian, China. Performed microtensile bond strength test.
c Dentist,
Department of Prosthodontics, School of Stomatology, Fourth Mili-
tary Medical University, Xian, China. Proofread manuscript.
d Graduate Student, Department of Electronic Microscopy Center, Fourth
Military Medical University, Xian, China. Performed SEM observation of ad-
hesive/dentin interfaces.
e Professor
and Chair, Department of Prosthodontics, School of Stomatology,
Fourth Military Medical University, Xian, China. Idea.
Correspondence: Professor Ji-hua Chen, Department of Prosthodontics,
School of Stomatology, Fourth Military Medical University, Changle Xi Road
145, Xian, 710032, China. Tel/Fax: +86-29-84776329. e-mail: jhchen@
fmmu.edu.cn
T he ultimate goal of dentin bonding procedures is the
complete infiltration of adhesive into the interfibril-
lar spaces and the encapsulation of the collagen fibrils
in demineralized dentin. With the water-wet bonding
technique, the presence of water in the demineralized
dentin can prevent the collapse of collagen matrix. The
space that is occupied by water surrounding the noncol-
lapsed collagen fibers can then be infiltrated by resin
monomers to form the hybrid layer.
However, several authors have suggested that it may
be impossible for resin monomers to displace all the
water around the collagen fibrils and within the interfi-
brillar spaces.4 This results in a layer of residual water
over the collagen fibrils that can prevent intimate con-
tact between resins and collagen fibrils, leaving poorly
encapsulated collagen. Additionally, the discrepancy

Vol 13, No X, 2011 1


Li et al
between dentin demineralization and adhesive infiltra-
tion within the water-saturated demineralized dentin can
cause incompletely impregnated zones along the bottom
of hybrid layer.1,5,30 Therefore, part of the collagen fibrils
in the hybrid layer may be exposed and surrounded by
water. Those denuded or poorly encapsulated collagen
fibrils could be hydrolyzed slowly via endogenous matrix
metalloproteinases (MMPs),9,10,15 raising a real concern
about the durability of bonding to water-saturated dentin.
Thus, procedures that improve resin infiltration by coating
each collagen fibril with resin may deny collagen-bound
MMPs access to water and make resin-dentin bonds more
durable.
Accordingly, an ethanol-wet bonding technique has
been proposed,14,20,25 in which ethanol instead of water
is used to support the demineralized dentin collagen ma-
trix. The spaces between the microfibrils are filled with
ethanol, which is a much better solvent for resin mono-
mers and may promote the intimate coating of adhesive
on collagen. Moreover, ethanol has been demonstrated
to decrease collagen fibrillar diameter and increase in-
terfibrillar space in hybrid layers,7 thus facilitating the
infiltration of resin monomers. Consequently, this tech-
nique can provide better resin sealing of the collagen
matrix24 and reduce the permeability of resin-dentin
bonding interface,2 thereby diminishing collagenolytic
activities of endogenous enzymes and improving the
bonding durability to dentin. It has commonly been sug-
gested to use the ethanol-wet bonding technique with
experimental hydrophobic adhesives,7,14,18,20,25 aiming
to both provide superior encapsulation of collagen with
bis-GMA infiltration and improve the resistance of the ad-
hesive interface to hydrolytic attack. Usually, the ethanol
saturation is achieved using a series of ascending etha-
nol concentrations, taking approximately 3 or 4 min-
utes, which defies the principles of user friendliness and
technique simplification.28 To overcome this obstacle,
simplified dehydration protocols applying 100% ethanol
once or three times were tested, but failed to generate
desirable results, due to the inadequate replacement of
water within the acid-etched dentin by ethanol. Since the
combination of ethanol-wet bonding and hydrophobic ad-
hesive is not optimal for clinical practice at present, the
contemporary dental adhesives containing hydrophilic
monomers, albeit unreliable in bonding stability, still
prevail clinically.
Most of the dental adhesives currently available on the
market are combinations of hydrophobic and hydrophilic
monomers. The hydrophobic components of adhesive are
well miscible with ethanol and the so-called hydrophilic
monomers also display better solubility in ethanol than
in water.22 Therefore, it is possible that these dental ad-
hesives may exhibit enhanced penetration in ethanol-wet
demineralized dentin matrix. Moreover, compared with hy-
drophobic adhesives, the contemporary hydrophilic ones
should be more tolerant to the presence of residual water
after ethanol wetting in a simplified dehydration protocol,
showing the potential for use in clinical practice. However,
the hypothesis that the hydrophilic adhesive could exhibit
enhanced performance with ethanol-wet bonding in a clini-
2 The Journal of Adhesive Dentistry
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cally acceptable dehydration period needs to be explored, lica
since little information is available on the bonding efficacy tio
te ot n
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and interfacial structure of current hydrophilic adhesives
sse nc e
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with ethanol-wet bonding.
In the present study, three commercially available etch-
and-rinse adhesives were applied to acid-etched dentin
with the water- or ethanol-wet bonding technique. The
objectives were to determine if bonds made with the eth-
anol-wet technique in a clinically acceptable dehydration
period are stronger and more durable than those made
with the water-wet bonding technique, and to explore the
possible reasons for the bonding results in terms of the
wettability of water/ethanol-saturated demineralized den-
tin matrix and the morphology of the hybrid layer. The null
hypothesis tested was that the water- and ethanol-wet
bonding techniques exhibited no differences in bonding
strength and durability for three contemporary etch-and-
rinse adhesives.
Materials and Methods
Tooth Preparation
Forty-eight third molars were collected after the do-
nors informed consent was obtained under a protocol
approved by the Fourth Military Medical University. The
roots of the teeth were removed 2 to 3 mm below the
cementoenamel junction by means of a water-cooled
low-speed saw (SYJ-150; MTI; Shenyang, China). Then
a flat surface was prepared by removing the occlusal
third of the tooth crowns with the saw to expose mid-
coronal dentin. The dentin surface was polished with
600-grit SiC paper to create a standardized smear
layer. The crown segments were randomly allocated to
6 groups (n = 8), according to the bonding techniques
(water-wet bonding vs ethanol-wet bonding) and the
three etch-and-rinse adhesives tested, Single Bond
2 (SB) (3M ESPE; St Paul, MN, USA), Prime & Bond
NT (PB) (Dentsply DeTrey; Konstanz, Germany), and
Gluma Comfort Bond (GB) (Heraeus Kulzer; Hanau,
Germany) (Table 1).
Bonding Procedure
According to the instructions of bonding adhesives, the
exposed dentin surfaces were acid etched with the cor-
responding etchants for 15 s, rinsed with water, and
then inverted on wet lint-free tissues until bonded.
For the water-wet bonding groups, two applications of
adhesive were made on the blotted water-moist dentin
surface and gently agitated with a microbrush for 10 s.
After resin infiltration, excess solvent was evaporated
with a gentle air stream for 10 s.The adhesive was
then light cured for 20s.Resin composite buildups were
constructed with 2-mm increments of Z250 (3M ESPE;
St Paul, MN, USA).
For the ethanol-wet bonding groups, the etched dentin
surface was inverted into 100% ethanol for 1 min, never
allowing the ethanol-saturated dentin to evaporate to dry-

Table 1 Adhesives tested in this study
Adhesive Composition
Single Bond 2, (SP) Etchant: 3M etchant
3M ESPE; St Paul, USA Adhesive: dimethacrylates, HEMA, polyalkenoid acid copolymer, 5 nm si-
lane treated colloidal silica, ethanol, water, photoinitiators
Prime & Bond NT (PB) Etchant: Caulk 34% Tooth Conditioner Gel
Dentsply DeTrey; Kon- Adhesive: di- and trimethacrylate resins, functionalized amorphous silica,
stanz, Germany PENTA, photoinitiators, cetylamine hydrofluoride acetone
Gluma Comfort Bond Etchant: Gluma Etch 20 Gel-phosphoric acid
(GB) Adhesive: HEMA, 4META, polyacid, photoinitiators, polyacrylic acids, etha-
Heraeus Kulzer; Hanau, nol, water
Germany
HEMA: 2-hydroxyethyl methacrylate; PENTA: dipentaerythritol penta acrylate monophosphate; 4META: 4-methacryloxyethyl trimellitic anhydride.
ness, thereby avoiding the surface tension forces. Then,
excess ethanol was blotted and the adhesive application
was performed as described above, followed by the con-
struction of composite buildups.
Specimen Preparation and Aging Procedures
After storage in de-ionized water at 37C for 24 h, each
tooth was vertically sectioned into 0.9-mm-thick serial
slabs by means of a saw (see above) with water cool-
ing. The central slab was utilized for subsequent mor-
phological examination. The other slabs were sectioned
into 0.9 x 0.9 mm composite-dentin beams, excluding
those situated peripherally that showed the presence
of enamel. Half of the beams in each group were imme-
diately subjected to microtensile bond strength testing;
the other half were immersed in 10% sodium hypochlo-
rite (NaOCl) solution (Kermel Chemical Reagent; Tianjin,
China) for 2 h and then tested for microtensile bond
strength. The protocol of reducing the specimens into
small sticks and immersing them in NaOCl solution for
a relatively short time period represents a form of ac-
celerated aging,12,21 to determine how well the resin
monomers protect the collagen matrix from proteolytic
degradation.12,33
Microtensile Bond Strength Testing
The beams from each group were subjected to tensile
testing. Each beam was stressed to failure under ten-
sion in a universal testing machine (EZ Test, Shimadzu;
Kyoto, Japan) at a crosshead speed of 1 mm/min. The
cross-sectional area at the site of failure was measured
with a pair of digital calipers (605-01, Links, HMCT; Har-
bing, China) to calculate the microtensile bond strength
values (MPa).
SEM Analysis of Hybrid Layer
The central slabs from each group were polished,
treated with the 37% phosphoric acid gel for 15 s, fol-
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Application steps e n
Etch for 15 s.
Rinse with water.
Keep dentin moist with water or
ethanol.
Apply 2 consecutive coats of the
adhesive.
Air thin.
Irradiate for 20 s.
Construct resin buildups.
lowed by 5.25% NaOCl for 10 min, to bring the resin/
dentin interfaces into relief. After water rinsing, the
specimens were then dehydrated using increasing con-
centrations of ethanol starting with 50%, 70%, and 85%
for 15 min each, followed by 100% ethanol for 30 min.
After drying in 100% ethanol overnight, the prepared
specimens were sputter coated with pure gold and
examined by means of SEM (Hitachi S-3400N; Tokyo,
Japan) at an accelerating voltage of 5 kV.
Wettability of Water- vs Ethanol-saturated Dentin
Fifteen third molars were processed by removing the
occlusal third and the apical third of the crowns with
the slow-speed saw under water cooling. The residual
crown segment was divided into two disks of midcoro-
nal dentin and the upper dentin disk was inverted to
expose the midcoronal dentin as the testing surface,
thus achieving two identical specimens from one tooth.
Two disks from one tooth were randomly allocated
into the water-saturated dentin group (n = 15) and the
ethanol-saturated dentin group (n = 15). Three kinds
of etch-and-rinse adhesives were used as reference
liquids to evaluate the contact angle as the wettability
index of the dentin disk. For each bonding adhesive,
10 dentin disks prepared from five teeth were acid
etched with the proprietary etchant for 15 s, rinsed
with water, and then either kept water-moist to obtain
water-saturated dentin (n = 5) or immersed in ethanol
as mentioned above to obtain ethanol-saturated dentin
(n = 5).
Droplets of each adhesive were placed on the dentin
disks using a microsyringe. The profiles of the droplets
were recorded for 60 s with a camera connected to a
goniometer (FM40, Krss; Hamburg, Germany) and an-
alyzed using drop shape analysis software (DSA1v1.9,
Krss) to calculate the contact angles with a frequency of
one reading every 1 s.6 One droplet of the adhesive was
applied on each specimen. Then five droplets on water-
saturated dentin and five droplets on ethanol-saturated
dentin were analyzed for each adhesive.

Li et al
Table 2 Microtensile bond strengths for water-wet and ethanol-wet bonding techniques
Adhesive 24-hour evaluation (MPa)
Water-wet
SB 32.4 (8.3)a
PB 27.2 (6.9)b
GB 27.8 (6.8)b
Bond strength values are means (standard deviation) in MPa, n = 40. Values identified with different superscript letters are signifi-
cantly different at p < 0.05. SB: Single Bond 2 ; PB: Prime Bond NT; GB: Gluma Comfort Bond.
Concentration of Nonvolatile Ingredients in Dental
Adhesives
An aliquot of each adhesive (approximately 150 l) was
added into a centrifuge tube, the weight of which was
recorded as W0. After weighing the system (W1), the
weight of the adhesive aliquot (Wa) was calculated with
the following formula: Wa = W1-W0. In subdued light, the
adhesive aliquot was spread onto an absorbent paper, the
weight of which was termed W2. After resin infiltration, the
solvent was evaporated with a gentle air stream for 1 min.
The resin absorbed in the absorbent paper was irradiated
for 20 s and then weighed together with the paper (W3).
The net weight of the nonvolatile ingredients (Wn) was cal-
culated as Wn = W3-W2. The concentration of nonvolatile
ingredients (Cn) in the dental adhesive was evaluated with
the following formula: Cn = (Wn/Wa) x 100%. Three inde-
pendent tests were carried out for each adhesive.
Statistical Analysis
All data collected from this research were first checked
for normal distribution with the Kolmogorov-Smirnov test
and tested for homogeneity with Levenes test. The ten-
sile strength data were analyzed using three-way ANOVA
(adhesive, bonding technique, and NaOCl challenge as
fixed factors) and Tukeys honestly significant difference
test. The contact angle data at each measurement time
and the thicknesses of hybrid layers were both analyzed
by two-way ANOVA (adhesive and bonding technique as
fixed factors) and Tukeys honestly significant difference
test. Statistical analyses were performed by SPSS 13.0
software (SPSS; Chicago, IL, USA) at a significance level
of p < 0.05.
Results
Microtensile Bond Strength (TBS) with the Two
Bonding Techniques
Mean bond strengths in MPa obtained for each group
are shown in Table 2. Mean bond strength was affected
by the adhesive system (F = 21.96; p < 0.001), bond-
ing technique (F = 44.89; p < 0.001) and NaOCl chal-
lenge (F = 759.75; p < 0.001).
4 The Journal of Adhesive Dentistry
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NaOCl challenge (MPa)
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Ethanol-wet Water-wet Ethanol-wet
37.3 (8.6)c 15.3 (4.2)d,e 19.3 (3.9)f
30.2 (7.8)a,b 14.0 (3.7)d 17.0 (3.9)e
31.5 (6.9)a,b 13.5 (3.5)d 16.7 (3.1)e
Mixed results were produced when three kinds of etch-
and-rinse adhesives were applied to acid-etched dentin
with the water-wet bonding technique. The 24-h bond
strength created by SB was the highest of all three ad-
hesives (p < 0.05), while no significant difference was
found between the other two adhesives (p > 0.05). The
subsequent chemical challenge with NaOCl statistically
decreased the TBS of all three adhesives (p < 0.05);
the TBS values of three groups showed no statistical
difference after NaOCl challenge (p > 0.05).
When adhesives were applied to ethanol-saturated
dentin, the 24-h bond strength of SB was significantly
higher than the value of the water-wet bonding technique
(p < 0.05), while the TBS of the other two adhesives
remained at the same levels as their counterparts with
the water-wet bonding technique (p > 0.05). After NaOCl
challenge, the TBS values of all three adhesives tended
to decrease (p < 0.05), but were still significantly higher
when compared with the data from the water-wet bonding
technique (p < 0.05).
SEM Observations
Representative SEM micrographs of the adhesive/den-
tin interface of specimens with water-wet or ethanol-wet
bonding are shown in Fig 1. An acid-resistant adhesive-
infiltrated layer and adhesive tags were clearly observed.
For the specimens of water-wet bonding, the layers were
porous and uneven, indicating that the quality of those
layers was low from the acid/NaOCl treatment. The thick-
nesses of the resin-infiltrated layers were 5.6 0.5 m
for SB specimens (n = 4), 5.1 0.5 m for PB (n = 4)
and 4.9 0.7 m for GB (n = 4). For the specimens of
ethanol-wet bonding, the well-defined, resin-infiltrated
layer thicknesses were 6.7 0.4 m for SB (n = 4),
5.5 0.7 m for PB (n = 4) and 5.6 0.5 m for GB
(n = 4), which were wider than those of water-wet bond-
ing specimens. The hybrid thickness differed statistically
significantly between the water-wet and ethanol-wet bond-
ing specimens of the SB group (p < 0.05).
Contact Angles of Dental Adhesive on Water- or
Ethanol-saturated Dentin
The contact angles of the three adhesives on water/
ethanol-saturated dentin are presented in Fig 2 and
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Water-wet bonding lica
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Single Bond 2 Prime Bond NT Gluma confort bond

Ethanol-wet bonding
Fig 1 SEM micrographs (magnification 3000X) of the adhesive/dentin interfaces with water-wet or ethanol-wet bonding. A, B and
C depict the adhesive/dentin interfaces of water-wet bonding for SB, PB and GB, respectively. Porous and uneven hybrid layers are
evident in these three micrographs. D, E and F depict the adhesive/dentin interfaces of ethanol-wet bonding for SB, PB and GB,
respectively, showing well-defined, resin-infiltrated layers. SB: Single Bond 2 ; PB: Prime Bond NT; GB: Gluma Comfort Bond. HL:
hybrid layer.

Table 3 Contact angle of dental adhesive on water-saturated or ethanol-saturated dentin at three measurement times

Contact angle on water-wet dentin (degrees) Contact angle on ethanol-wet dentin (degrees)
Reference liquid
Initial 20 s Final Initial 20 s Final
SB 38.4 (4.0)a 26.8 (2.0)c 23.4 (2.9)e 31.8 (4.3)g 20.3 (1.9)h 18.1 (1.6)j

PB 30.3 (3.3)b 18.7 (2.2)d 16.1 (1.9)f 29.9 (3.5)g 14.5 (2.7)i 12.7 (2.2)k

GB 33.5 (1.6)b 19.6 (3.5)d 16.7 (2.2)f 31.1 (2.3)g 15.9 (1.4)i 13.5 (0.5)k

Contact angle values are means (SD), n = 5. Values designated with different superscript letters at each measurement time are significantly different at
p < 0.05. SB: Single Bond 2 ; PB: Prime Bond NT; GB: Gluma Comfort Bond.

Table 3. Regardless of the solvent used to saturate the
etched dentin, the contact angles between the dentin
and the reference liquid decreased over time. At each
measurement time throughout the kinetic study, for
each adhesive, ethanol-saturated dentin exhibited lower
contact angles that did water-saturated dentin. The dif-
ference in the SB group was even greater, achieving sig-
nificantly different contact angles at each measurement
time (0.01 < p < 0.40); for PB and GB, contact angles
on ethanol-saturated specimens were almost equivalent
to those of water-saturated specimens immediately
after drop application, and then the contact angle kinet-
ics evolved rapidly for ethanol-saturated specimens,
leading to significantly lower contact angles on ethanol-
saturated dentin specimens after 11 s and 33 s
(p < 0.05). Moreover, regardless of the adhesive used
as reference liquid, the contact angle kinetic curves
for ethanol-saturated specimens decreased rapidly and
then flattened beyond 20 s, which different from the
relatively smooth curves of water-saturated groups.
When comparing the three adhesives, SB presented
the highest contact angle initially, 20 s after application,
and at the final time point on water-saturated dentin, as
well as at 20 s after application and the final time point

Vol 13, No x, 2011 5


Li et al
40
35
Contact Angle ()
30
25
20
15
10
0 10 20 30 40 50 60
Time (sec)
on ethanol-saturated dentin (p < 0.05), while between the
other two adhesives, a statistically significant difference
could not be detected at these three measurement times
either on water- or ethanol-saturated dentin (p > 0.05).
Concentration of Nonvolatile Ingredients in Dental
Adhesives
The concentrations of nonvolatile ingredients varied
among three adhesives, with 68.1 1.2% for SB,
33.7 0.6% for PB, and 49.5 0.9% for GB.
Discussion
The ongoing problems associated with dental adhe-
sives, such as poor durability of dentin bonding, could
be partially attributed to the poor infiltration and en-
capsulation of wet dentin with adhesive monomers.
The resultant hybrid layer would be suboptimal and
more prone to hydrolytic degradation. Since ethanol is
a desirable solvent for most hydrophobic monomers,
the ethanol-wet bonding technique has been proposed
to be used with hydrophobic adhesives to enhance the
infiltration of adhesive monomers and reduce the degra-
dation of the bonded interface.24 Although they exhibit
excellent bond strength and favorable bond durability,
hydrophobic adhesives are still less optimal for clini-
cal application at present due to the time-consuming
dehydration procedure of ethanol-wet bonding. Dental
adhesives containing hydrophilic monomers, albeit unre-
liable in terms of bonding stability, still prevail clinically.
6 The Journal of Adhesive Dentistry
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SB/ethanol-wet dentin tio
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SB/water-wet dentin
PB/ethanol-wet dentin
PB/water-wet dentin
GB/ethanol-wet dentin
GB/water-wet dentin
Fig 2 Contact angle kinetics
of dental adhesive on water-
saturated or ethanol-saturated
dentin. At each measurement
time for each adhesive, etha-
nol-saturated dentin exhibited
a lower contact angle than did
water-saturated dentin. For
group abbreviations, see Fig 1.
In contemporary dental adhesives, high concentrations
of relatively hydrophilic monomers (eg, HEMA in SB and
GB, PENTA in PB) are generally blended with hydropho-
bic adhesive monomers (eg, bis-GMA, UDMA). Whether
they can provide acceptable bonding when used with
the ethanol-wet bonding technique in a clinically accept-
able dehydration period is still unknown.
To address this issue, we evaluated the effect of the
ethanol-wet bonding technique on the bond strength and
durability of three adhesives containing hydrophilic mono-
mers with a simplified dehydration protocol. The results
indicated that compared with water-wet bonding, etha-
nol-wet bonding mediated a similar or higher 24-h bond
strength with the dental adhesives tested, and displayed
enhanced bonding durability against chemical challenge.
The findings led to partial rejection of the null hypothesis,
that the water- and ethanol-wet bonding techniques exhib-
ited no differences in the bonding strength and durability
for the three etch-and-rinse adhesives tested.
Hoys solubility parameter theory has been used to
predict the miscibility of two different solutions by com-
paring their total cohesive energy (t) values. It predicts
that if there is less than 5 (J/cm3)1/2 between the t
values of a solution and a second solution or a substrate,
the solution will wet the substrate and cause it to swell
enough to permit entry of the solution.27 Information on
the exact ingredients of the dental adhesives used in
this study was not available to us to calculate their Hoys
values. However, previous studies which listed the Hoys
values of some experimental adhesives reported that
the Hoys t values of hydrophilic adhesives were in the
range of 21.1 to 24.2 (J/cm3)1/2.7,22 Since the Hoys t
values for water-saturated and ethanol-saturated collagen

matrix are 30.1 and 25.1 (J/cm3)1/2, respectively,7,14 we
could speculate that the hydrophilic adhesive might have
better miscibility with ethanol-saturated collagen matrix,
thus leading to better resin infiltration and stronger bond
strength, as indicated in this study.With ethanol-wet bond-
ing, an excess of ethanol replaces water in the interfibril-
lar spaces and at the top of the dentinal tubules, as etha-
nol is completely miscible with water. Since ethanol is a
desirable solvent for most hydrophobic monomers and
a better solvent for the so-called hydrophilic monomers
than water,22 modern adhesives which contain a blend of
hydrophilic and hydrophobic monomers may then be able
to infiltrate closely around collagen fibrils into the area
which was occupied by the residual layers of ethanol,
therefore producing an optimal encapsulation of collagen
with adhesive resin and inactivating the collagen-bound
endogenous MMPs. Conversely, with water-wet bonding,
the presence of residual water around collagen fibrils may
cause micro- or nanophase separation of dentin adhe-
sives,3,29,31 thus inducing incomplete monomer polym-
erization around collagen fibrils and generating porosities
within bonded interfaces.
Apart from providing better solubility of adhesive
resin, ethanol is also capable of collapsing the prote-
oglycan hydrogel which is claimed to clog the collagen
matrix13,17 and interfere with resin infiltration.23 Moreo-
ver, ethanol has been demonstrated to shrink the diam-
eter of collagen fibrils more than it shrinks the volume of
the matrix,7,25 thereby enlarging the interfibrillar spaces
and allowing for more resin infiltration. Accordingly, with
ethanol-wet bonding adhesive resin may penetrate into
the deep zone of collagen network and establish an op-
timal hybrid layer. This is unlikely to occur for water-wet
bonding samples, since the relatively poor impregnation
of monomers into the water-saturated collagen matrix
might leave nude collagen fibrils along the bottom of the
hybrid layer.1,5,30
Accordingly, the ethanol-wet bonding technique may
ensure an intimate association between collagen fibers
and resin, which could protect collagen fibers from hy-
drolysis. Moreover, adhesive resin can penetrate deeper
into ethanol-saturated dentin matrix to form a well-de-
fined, wider resin-infiltrated layer, as demonstrated in
our SEM observations. These may be responsible for
the higher resin-dentin bond strength and better bonding
durability of ethanol-wet bonding compared with water-
wet bonding.
Although the ethanol-bonding group of each adhesive
tested in the present study yielded higher 24-h bonding
strength than its water-bonding counterpart, only SB
exhibited a statistical difference between two bonding
techniques, presumably because the penetration ability
of SB into these two different solvent-saturated dentin
matrices differs dramatically. Compared with the other
two adhesives, the high percentages of nonvolatile ingre-
dients in SB and the introduction of colloidal silica in its
composition might compromise its flowability and wet-
ting effect on water-saturated dentin matrix. However,
when applied to ethanol-saturated dentin, the wetting
ability of SB improved greatly as indicated in contact
Vol 13, No x, 2011 7
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ub
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angle measurements, which would facilitate the infil- lica
tration of resin into collagen matrix and subsequently tio
te n
ot
n
improve the 24-h bonding strength significantly. Con-
sse nc e
fo r
versely, for the other two adhesives, the relatively higher
concentration of adhesive solvent enhanced their wet-
ting ability on water-saturated dentin. Especially for PB,
an acetone-solvated adhesive, the azeotrope effect11
or water-chasing effect8 of acetone can lead to bet-
ter evaporation of water, rendering this adhesive better
able to penetrate into water-saturated dentin. Therefore,
ethanol-wet bonding could only improve the 24-h bonding
strengths of PB and GB slightly, and the positive effect
of ethanol-wet bonding on bonding efficacy might be
influenced by the composition and resin concentration
of contemporary adhesives.
The difference in concentrations of nonvolatile in-
gredients, mostly resin monomers, among these three
adhesives may also provide an explanation for their dif-
ferent bond strengths and hybrid layer thicknesses. The
water-saturated or ethanol-saturated dentin matrix is
compliant and can easily shrink when the solvent is
evaporated.14 The more concentrated the monomer is,
the less the matrix shrinks when the solvent is evapo-
rated, resulting in higher net monomer uptake.14 Thus,
higher net resin uptake might be expected for SB speci-
mens, since this adhesive has a higher concentration
of nonvolatile ingredients, therefore providing greater
bond strength and thicker hybrid layer than the other
two adhesives.
An important concern about ethanol-wet bonding is
that the protocol is time consuming and technique sen-
sitive.19 In the current study, the ethanol-wet bonding
technique was performed over a more clinically relevant
time period (1 min), and exhibited encouraging results
with contemporary hydrophilic etch-and-rinse adhesives.
However, it is questionable that simplified dehydration
protocols might actually lead to incomplete water replace-
ment, hence impairing the bonding efficacy of hydropho-
bic adhesives. Due to the existence of a small amount of
residual water, this dentin matrix should have a Hoys t
value somewhere between 25.1 and 30.1 (J/cm3)1/2 (the
Hoys t values for water-saturated and ethanol-saturated
collagen matrix, respectively), therefore enlarging its dis-
crepancy with the Hoys t value of hydrophobic adhesive.
Conversely, for the hydrophilic etch-and-rinse adhesives
tested, their Hoys t values were higher than that of hy-
drophobic adhesive, therefore generating a smaller t
value with this dentin matrix and leading to better mis-
cibility of these two entities. This indicates that contem-
porary hydrophilic adhesives should be more tolerant to
the presence of residual water in the ethanol-wet dentin
matrix and exhibit desirable bonding performance with the
simplified dehydration protocol.
However, the residual water in the dentin matrix and
the hydrophilic domains of contemporary dental adhe-
sives will make the hybrid layer behave as semi-permea-
ble membranes, which permits water movements through
the bonded interface even after the adhesive is polymer-
ized.26 Hydrolysis can subsequently occur in the resin and
collagen of the hybrid layer and compromise the long-term

Li et al
References
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Acknowledgments
We gratefully acknowledge the scanning electron micro-
scope center of the Fourth Military Medical University
for technological support and providing equipment. This
research work was financially supported by a grant (No.
30901695) from the Natural Science Foundation of
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Clinical relevance: The use of the ethanol-wet bonding
technique in a clinically acceptable dehydration period
might improve the bonding efficacy of contemporary
hydrophilic adhesives and could be an alternative for
their clinical application.

Vol 13, No x, 2011 9

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