Influence of Application Time and Etching Mode of

Universal Adhesives on Enamel Adhesion

Keiichi Saia / Toshiki Takamizawab / Arisa Imaic / Akimasa Tsujimotod / Ryo Ishiie / Wayne W. Barkmeierf /
Mark A. Lattag / Masashi Miyazakih

Purpose: To investigate the influence of application time and etching mode of universal adhesives on enamel adhesion.
Materials and Methods: Five universal adhesives, Adhese Universal, Bondmer Lightless, Clearfil Universal Bond
Quick, G-Premio Bond, and Scotchbond Universal, were used. Bovine incisors were prepared and divided into four
groups of ten teeth each. SBS, Ra, and SFE were determined after the following procedures: 1. self-etch mode with
immediate air blowing after application (IA); 2. self-etch mode with prolonged application time (PA); 3. etch-and-rinse
mode with IA; 4. etch-and-rinse mode with PA. After 24-h water storage, the bonded assemblies were subjected to
shear bond strength (SBS) tests. For surface roughness (Ra) and surface free energy (SFE) measurements, the adhe-
sives were simply applied to the enamel and rinsed with acetone and water before the measurements were carried
out.
Results: Significantly higher SBS and Ra values were obtained with etch-and-rinse mode than with self-etch mode re-
gardless of the application time or type of adhesive. Although most adhesives showed decreased SFE values with in-
creased application time in self-etch mode, SFE values in etch-and-rinse mode were dependent on the adhesive type
and application time.
Conclusions: Etching mode, application time, and type of adhesive significantly influenced the SBS, Ra, and SFE
values.
Keywords: universal adhesive, etching mode, application time, enamel bond efficacy.

J Adhes Dent 2018; 20: 65–77. Submitted for publication: 18.11.17; accepted for publication: 07.02.18
doi: 10.3290/j.jad.a39913

D ental adhesives comprised of a combination of com-

posites are constantly being improved to overcome
their shortcomings, and to expand the range of clinical ap-
plications for anterior as well as posterior lesions.25 The
latest generation of adhesives are referred to as “universal
adhesives” and have been extensively implemented due to
their versatility.5,15 Universal adhesives are thought to pro-
vide benefits to clinicians owing to their simplified bonding
steps and broad applicability in numerous clinical situa-
tions. One of the most important expectations for universal
adhesives is that the adhesives can be used with either
self-etch or etch-and-rinse modes.9,14 This multimode
usage of universal adhesives has been reported to enhance
enamel bond durability with an etch-and-rinse approach and
reduce damage to dentin with a self-etch approach.19,20
Thus, practitioners should select the optimal etching mode
when using universal adhesives in accordance with cavity
features such as depth, size, location, and proportions of
enamel and dentin. In addition, universal adhesives can be
used not only for direct composite restorations but also for

a Graduate Student, Department of Operative Dentistry, Nihon University School of
Dentistry, Tokyo Japan. Performed experiments (bond strength test and surface
roughness measurement), statistical evaluations, and contributed to discussion.
b Associate Professor, Department of Operative Dentistry, Nihon University
School of Dentistry, Tokyo Japan. Idea, hypothesis, experimental design, wrote
the manuscript, and discussed the results at all stages.
c Graduate Student, Department of Operative Dentistry, Nihon University School
of Dentistry, Tokyo Japan. Performed experiments (surface free measurement).
d the manuscript at all stages.
Assistant Professor, Department of Operative Dentistry, Nihon University
School of Dentistry, Tokyo Japan. Consulted on statistical evaluation and con-
tributed to discussion.
e Postdoctorol Fellow, Department of Operative Dentistry, Nihon University
School of Dentistry, Tokyo Japan. Performed experiments (SEM observations)
and statistical evaluations.
f Adjunct Professor and Dean Emeritus, Department of General Dentistry,
Creighton University School of Dentistry, Omaha, NE, USA. Proofread the man-
uscript, contributed to discussion.
g Professor and Dean, Department of General Dentistry, Creighton University
School of Dentistry, Omaha, NE, USA. Proofread the manuscript, contributed
to discussion.
h Professor and Chair, Department of Operative Dentistry, Nihon University
School of Dentistry, Tokyo Japan. Discussed the results and commented on
Correspondence: Dr. Toshiki Takamizawa, Department of Operative Dentistry,
Nihon University School of Dentistry, 1-8-13, Kanda-Surugadai, Chiyoda-Ku,
Tokyo 101-8310, Japan. Tel: +81-3-3219-8141;
e-mail: takamizawa.toshiki@nihon-u.ac.jp

Vol 20, No 1, 2018 65

Sai et al

Table 1 Materials used in this study

Code Adhesive Manufacturer Main components

GP G-Premio Bond GC; Tokyo, Japan MDP, 4-MET, MEPS, BHT, acetone, dimethacrylate resins,
(4G0011) initiators, water

SU Scotchbond Universal 3M Oral Care; St Paul, MN, MDP, HEMA, dimethacrylate resins, Vitrebond copolymer, filler,
(41256) USA ethanol, water, initiators, silane

AU Adhese Universal Ivoclar Vivadent; Schaan, MDP, bis-GMA, HEMA, MCAP, D3MA, ethanol, water, initiator,
(U49302) Lichtenstein stabilizers, silicon dioxide

CQ Clearfil Universal Quick Kuraray Noritake; Tokyo, bis-GMA, MDP, HEMA, hydrophilic amide monomer, filler,
(9T0050) Japan ethanol, water, NaF, photo initiators, chemical polymerization,
accelerator, others

BM Bondmer Lighless Tokuyama Dental; Tokyo, Liquid A: phosphate monomer, bis-GMA, TEG-DMA, HEMA,
(004067) Japan MTU-6, others
Liquid B: acetone, isopropanol, water, acryl borate catalyst,
-MPTES, peroxide, others

Pre-etching agent Manufacturer Main components

Ultra-Etch Ultradent 35% phosphoric acid
(G017)

Composite Manufacturer Main components

Clearfil AP-X Kuraray Noritake Dental Bis-GMA, TEG-DMA, silane barium glass filler, silane silica
(N416713) filler, silanated colloidal silica, CQ, pigments, others

MDP: 10-methacryloyloxydecyl dihydrogen phosphate; 4-MET: 4-methacryloxyethyl trimellitate; MEPS: methacryloyloxyalkyl thiophosphate methylmethacrylate;
BHT: butylated hydroxytoluene; HEMA: 2-hydroxyethyl methacrylate; bis-GMA: 2,2-bis[4-(2-hydroxy-3- methacryloyloxypropoxy) phenyl) propane; MCAP:
methacrylated carboxylic acid polymer; D3MA: decandiol dimethacrylate; TEG-DMA: triethyleneglycol dimethacrylate; MTU-6: 6-methacryloyloxyhexyl-2-thiouracil-
5-carboxylate; J-MPTES: J-methacryloyloxypropyltriethoxysilane; CQ: dl-camphorquinone.

indirect ceramic restorations.24 Universal adhesives are ex-
pected to help simplify the bonding procedure for patch res-
torations when used to repair aged restorations with flaws
on the surface. Although the versatility of universal adhe-
sives has been documented, care should be taken because
not all universal adhesives have the same characteristics
and clinical usage may differ with regard to obtaining opti-
mal bonding performance.
Over the past few years, many manufacturers have intro-
duced different types of universal adhesives, a recent trend
being the introduction of reduced application time to the ad-
herent surface before light irradiation of the adhesive.17
Manufacturers advertise the lack of waiting periods and the
ability to achieve bonding by air blowing on the surface to
which adhesive has been applied. On the other hand, the
bonding efficacy of self-etch adhesives critically depends on
the chemical reaction between functional monomers and hy-
droxyapatite (HAp).26,27 This chemical interaction is thought
to form stable monomer-calcium salts and also to enhance
the bonding performance of self-etch adhesives.28 However,
the question still remains whether the shortened application
time is sufficient to create an adequate chemical bond. Little
information is available on the effect of the application-time
sensitivity of universal adhesives on bonding efficacy and
the chemical reaction with HAp in different etching modes.
In order to grasp the bonding performance of adhesives,
bond strength tests are widely employed with established
methods.6 However, to obtain a deeper understanding of the
bonding mechanism, other methodologies that focus on the
physical and chemical interactions between the adhesive
and mineralized tissues are necessary. Surface free energy
(SFE) determination with contact angle measurements is
one of the methods used to investigate the chemical interac-
tions between adhesives and mineralized tissues.10,25
The purpose of the present study was to determine the
influence of reduced application time on the enamel bond
efficacy of universal adhesives with different etching
modes, based on bond strength tests, morphological obser-
vations, surface roughness, and SFE characteristics. The
null hypotheses examined were that reduced application
time would not affect the enamel bond strength or the SFE,
regardless of the etching mode.
MATERIALS AND METHODS
Study Materials
The materials used in this study are shown in Table 1. The
five universal adhesives used were: 1. Adhese Universal
(AU, Ivoclar Vivadent; Schaan, Liechtenstein); 2. Bondmer
Lightless (BM, Tokuyama Dental; Tokyo, Japan); 3. Clearfil
Universal Bond Quick (CQ, Kuraray Noritake; Tokyo, Japan);
4. G-Premio Bond (GP, GC; Tokyo, Japan); 5. Scotchbond
Universal (SU, 3M Oral Care; St Paul, MN, USA). The phos-
phoric acid etching agent used was Ultra-Etch (Ultradent;
South Jordan, UT, USA). Clearfil AP-X (Kuraray Noritake) was

66 The Journal of Adhesive Dentistry

 Sai et al

Table 2 Application protocol for pre-etching and self-etch adhesives

Method Pre-etching protocol

code
Etch-and- Enamel surface was conditioned with phosphoric acid for 15 s, then rinsed with water for 15 s with a three-way dental
rinse syringe and air dried.

Self-etch Phosphoric acid pre-etching was not performed.

Adhesive Application Adhesive application protocol

method
GP IA* Adhesive was applied to the air-dried enamel surface and immediately a strong stream of air was applied
over the liquid adhesive for 5 s or until the adhesive no longer moved and the solvent had completely
evaporated. Light irradiation was performed for 10 s.

PA Adhesive was applied to the air-dried enamel surface for 10 s and then a strong stream of air was
applied over the liquid adhesive for 5 s or until the adhesive no longer moved and the solvent had
completely evaporated. Light irradiation was performed for 10 s.

SU IA Adhesive was applied to the air-dried enamel surface and immediately medium air pressure was applied
over the liquid adhesive for 5 s. Adhesive was light cured for 10 s.

PA* Adhesive was applied to the air-dried enamel surface with rubbing action for 20 s and then medium air
pressure was applied to the surface for 5 s. Adhesive was light cured for 10 s.

AU IA Adhesive was applied to the air-dried enamel surface immediately medium air pressure applied over the
liquid adhesive for 5 s. Light irradiation was performed for 10 s.

PA* Adhesive was applied to the air-dried enamel surface with rubbing action for 20 s and then medium air
pressure was applied to the surface for 5 s. Light irradiate was performed for 10 s.

CQ IA* Adhesive was applied to the air-dried enamel surface and immediately medium air pressure was applied
over the liquid adhesive for 5 s or until the adhesive no longer moved and the solvent had completely
evaporated. Light irradiate was performed for 10 s.

PA Adhesive was applied to air-dried enamel surface for 10 s and then medium air pressure was applied
over the liquid adhesive for 5 s or until the adhesive no longer moved and the solvent had completely
evaporated. Light irradiation was performed for 10 s.

BM IA* Adhesive was applied to the air-dried enamel surface and then immediately medium air pressure was
applied over the liquid adhesive for 5 s. No light irradiation.

PA Adhesive was applied to the air-dried enamel surface for 10 s and then medium air pressure was applied
over the liquid adhesive for 5 s. No light irradiation.

IA: immediately air-blow after application of adhesive. PA: application of adhesive according to each manufacturer’s instructions (GP, SU, and AU) or
application of adhesive for 10 s (CQ and BM). * Manufacturer’s instructions.

used as a restorative material for bonding. To avoid any in-
fluence from the reported nonuniformity of LED curing
units,13,16 a halogen-quartz-tungsten curing unit was used,
specifically a visible-light curing unit (Optilux 501, SDS Kerr;
Danbury, CT, USA). The light irradiance (average 600 mW/
cm2) of the curing unit was checked using a dental radiom-
eter (Model 100, Kerr; Orange, CA, USA).
Specimen Preparation
Extracted mandibular bovine incisors stored frozen for up to
2 weeks were used. Approximately two-thirds of the apical
root structure of each tooth was removed using a diamond-
impregnated disk attached to a low speed saw (Isomet
1000, Low Speed Saw, Buehler; Lake Bluff, IL, USA). Pulp
tissues were then removed and the pulp chamber of each
tooth was filled with cotton. The labial surfaces were ground
with wet #240-grit silicon carbide (SiC) paper (Fuji Star Type
DDC; Saitama, Japan) to create a flat enamel surface. Each
tooth was mounted in self-curing acrylic resin (Tray Resin II;
Shofu; Kyoto, Japan) to expose the flattened area. The
enamel surfaces were polished using water cooling and a
sequence of silicon-carbide polishing papers ending with
400-grit SiC paper (Fuji Star Type DDC). Specimens were
prepared either in etch-and-rinse mode – in which phosphoric
acid was applied for 15 s prior to the application of the ad-
hesive – or in self-etch mode, ie, without phosphoric acid
etching. For each enamel surface, the adhesives were either
applied and immediately subjected to air blowing (immediate
air blow, IA) or the GP, SU, and AU adhesives were applied in
accordance with the manufacturer’s recommended applica-
tion time, whereas CQ and BM were applied for 10 s (pro-
longed application, PA). Air blowing was always carried out in
accordance with the manufacturer’s instructions (Table 2).
The experimental groups for all tests were all four combina-
tions of IA or PA with self-etch and etch-and-rinse modes, for
each adhesive, yielding a total of 20 groups.

Vol 20, No 1, 2018 67

Sai et al
Shear Bond Strength Tests
The shear bond strength (SBS) to enamel was measured
using the notched-edge SBS test as described in ISO
29022.11 The experimental protocols for the bonding proce-
dures are shown in Table 2. Ten specimens were used for
each test group. Ten specimens for each test group were
used to determine the enamel SBS in etch-and-rinse mode
or in self-etch mode. For each etched enamel surface, the
adhesives were either applied and immediately air blown
(immediate air blow, IA) or the GP, SU, and AU adhesives
were applied in accordance with the manufacturer’s recom-
mended application time, whereas CQ and BM were applied
for 10 s (prolonged application, PA). Air blowing was always
carried out in accordance with the manufacturer’s instruc-
tions (Table 2).
An Ultradent bonding assembly (Ultradent) was used for
determining SBS. Following application of the adhesive to
the adherent sites, a resin composite was placed into the
bonding mold inserts (2.4 mm in internal diameter, approxi-
mately 2.5 mm in height; Ultradent) on the enamel surfaces
using the bonding clamp (Ultradent), after which light irradia-
tion was performed for 30 s. The bonded specimens were
stored in distilled water at 37°C for 24 h and were then
loaded to failure at 1.0 mm per min with a test base clamp
(Ultradent) using a universal testing machine (Type 5500R,
Instron; Canton, MA, USA). The shear bond strengths (MPa)
were calculated from the peak load at failure divided by the
bonded surface area. After testing, the bonding site of the
tooth surfaces and resin composite cylinders were observed
under an optical microscope (SZH-131, Olympus; Tokyo,
Japan) at a magnification of 10X to determine the type of
bond failure. Based on the percentage of substrate area
observed on the debonded cylinders and tooth bonding
sites, failures were classified into four types: adhesive, co-
hesive in composite, cohesive in enamel, or mixed, ie, par-
tially adhesive and partially cohesive.
Surface Roughness Measurements
The specimens for surface roughness (Ra) measurement
were initially prepared using the same procedures de-
scribed above. In order to evaluate the exact etching ability
of each adhesive over different application times, the
enamel surfaces were polished using water coolant and a
sequence of silicon carbide polishing papers ending with
4000-grit SiC paper (Fuji Star Type DDC) to eliminate the
influence of scratches from polishing. Each enamel surface
was treated in accordance with the experimental protocol,
and the uncured adhesive layer was removed through three
alternating rinses each of acetone and water. Subse-
quently, the enamel surface was dried with oil-free com-
pressed air. Samples ground with wet 4000-grit SiC paper
with and without phosphoric acid pre-etching were also
measured as a baseline. The baseline samples were only
rinsed with water (not acetone).
The specimen surfaces after each treatment were ob-
served under a three-dimensional laser scanning micro-
scope (LSM VK-8700, Keyence; Osaka, Japan). The excita-
tion light had a spectral maximum of 658 nm and the light
68
intensity as well as the amplification of the photomultiplier
were kept constant during the observation period. The Ra
value was measured using the LSM proprietary software
(VK-Analyzer; Keyence), and each region of measurement
was 1.0 mm x 1.0 mm. The Ra was measured on 10 speci-
mens for each group at three regions as close as possible
to the center of the specimens, and the mean value was
determined for each group.
Surface Free Energy Measurements
The specimens used for measuring SFE were prepared as
described above. After application, the adhesives were re-
moved by rinsing with acetone and water, similar to the Ra
measurements. The prepared specimens were then used
for contact angle measurements to analyze the surface
characteristics of each treated enamel surface. Enamel
samples ground with wet #400-grit SiC paper with and with-
out phosphoric acid pre-etching were also measured as a
baseline.
The SFE values were determined by measuring the con-
tact angles on the surface using three test liquids as previ-
ously reported.10,25 The three test liquids used were 1-bro-
monaphthalene, diiodomethane, and distilled water. The SFE
parameters for the test liquids have been reported previ-
ously.10,25 The contact angle measurement equipment (Drop
Master DM 500, Kyowa Interface Science; Saitama, Japan)
was connected to a charge-coupled device camera, which
enabled automatic measurements of the contact angles.
For each test liquid, the equilibrium contact angle (T)
was measured using the sessile-drop method at 23 ± 1°C
in ten enamel specimens for each condition. Sessile drops
of each liquid were dispensed with a volume of 1.0 μl using
a micropipette. The SFE parameters for the solids were
then determined based on the fundamental concepts of
wetting. The Young-Dupré equation describes the work of
adhesion for a solid (S) and liquid (L) that are in contact
(WSL), the interfacial free energy between the solid and the
liquid (JSL), and the SFE of the liquid and solid (JL and JS,
respectively), as follows:
WSL = JL + JS–JSL = JL (1 + cosT)
by extending the Fowkes equation following the Kitazaki-
Hata approach:8
JSL = JL + JS–2 (JLd JSd)1/2–2 (JLp JSp)1/2–2 (JLh JSh)1/2
JL = JLd + JLp + JLh, JS = JSd + JSp + JSh
where Jd, Jp, and Jh are components of the SFE (J) arising
from the dispersion force, the polar (permanent and in-
duced) force, and the hydrogen-bonding force, respectively.
The T values were determined for the three test liquids, and
the surface energy parameters for the treated enamel sur-
faces were calculated based on the equations using add-on
software and the interface measurement and analysis sys-
tem (FAMAS, Kyowa Interface Science). The surface free
energy of the enamel was measured on 10 specimens for
each group and the mean value was determined.
The Journal of Adhesive Dentistry
 Sai et al

Table 3 Influence of application duration on enamel bond strength (MPa)

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 24.2 (2.3)bB 26.5 (1.8)aB 34.3 (2.0)bA 35.4 (2.8)cA

SU 21.6 (4.1)bC 28.3 (4.0)aB 43.2 (3.9)aA 38.9 (4.7)bcA

AU 23.8 (2.2)bC 29.1 (5.0)aB 44.7 (4.2)aA 40.5 (3.2)bA

CQ 25.0 (2.6)abB 27.1 (2.4)aB 47.0 (2.7)aA 47.5 (5.2)aA

BM 28.8 (4.4)aB 30.0 (5.1)aB 43.4 (1.5)aA 43.9 (2.1)abA

N = 10, mean (SD) in MPa. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital letters
in rows indicate no difference at the 5% significance level.

Table 4 Failure mode* analysis of debonded specimens

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 100/0/0/0 100/0/0/0 100/0/0/0 100/0/0/0

SU 100/0/0/0 100/0/0/0 80/0/10/10 90/0/0/10

AU 100/0/0/0 90/10/0/0 90/0/0/10 90/0/0/10

CQ 100/0/0/0 100/0/0/0 80/0/10/10 70/0/10/20

BM 90/10/0/0 100/0/0/0 80/10/0/10 80/0/20/0

*Failure modes in percent: adhesive failure/cohesive failure in resin composite/cohesive failure in enamel/mixed failure.

Table 5 Influence of application duration on surface roughness (Ra)

Baseline (4000 grit) Baseline (pre-etching)

0.097 (0.002)dB 0.097 (0.002)eB 0.741 (0.05)abA 0.741 (0.05)aA

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 0.194 (0.01)aC 0.231 (0.01)aB 0.692 (0.02)cA 0.697 (0.02)abA

SU 0.129 (0.01)bD 0.157 (0.01)cC 0.713 (0.01)bA 0.590 (0.02)cB

AU 0.126 (0.01)bcD 0.186 (0.01)bC 0.767 (0.02)aA 0.592 (0.01)cB

CQ 0.122 (0.01)bcC 0.122 (0.01)dC 0.656 (0.01)dB 0.688 (0.03)bA

BM 0.114 (0.01)cC 0.157 (0.01)cB 0.688 (0.02)cA 0.687 (0.01)bA

N = 10, mean (SD) in μm. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital letters
in rows indicate no difference at the 5% significance level.

Scanning Electron Microscopy Observations
Representative restorative/enamel interfaces and treated
enamel surfaces were observed in three samples using
field-emission scanning electron microscopy (SEM ERA-
8800FE, Elionix; Tokyo, Japan). For ultrastructural observa-
tions of the restorative/enamel interface, bonded samples
that had been stored in 37°C distilled water for 24 h were
embedded in epoxy resin and then longitudinally sectioned
with a low-speed saw (Isomet 1000). The sectioned sur-
faces were polished to a high gloss with abrasive disks (Fuji
Star Type DDC) followed by diamond pastes down to a par-
ticle size of 0.25 μm (DP-Paste, Struers; Ballerup, Den-
mark). For observation of the treated enamel surfaces,
specimens were treated in accordance with the experimen-

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Sai et al

100 Dispersion force

Polar force

Hydrogen-bonding force

80
Surface free energy (mN • m-1)

60

40

20

0
Baseline GP SU AU CQ BM
#400-grit
Phoshphoric acid etching

Self-etch mode IA

Self-etch mode PA
Etch-and-rinse mode IA
Etch-and-rinse mode PA

Self-etch mode IA

Self-etch mode PA
Etch-and-rinse mode IA
Etch-and-rinse mode PA

Self-etch mode IA
Self-etch mode PA
Etch-and-rinse mode IA
Etch-and-rinse mode PA

Self-etch mode IA
Self-etch mode PA
Etch-and-rinse mode IA
Etch-and-rinse mode PA

Self-etch mode IA
Self-etch mode PA
Etch-and-rinse mode IA
Etch-and-rinse mode PA
Fig 1 The total surface free energies result from different application times in different etching modes.

tal protocol and then rinsed with acetone and water similar ships between the tested parameters (SBS, Ra, and SFE),
to the Ra measurement. In addition, samples ground with the Pearson product-moment correlation coefficient was used
wet #400-grit SiC paper (Fuji Star Type DDC) with and with- for pairwise comparisons. To understand the correlation
out phosphoric acid pre-etching were examined as a base- among SBS, Ra and SFE values, the Pearson product-mo-
line. These samples were rinsed with water but not acetone. ment correlation coefficient was used for pairwise compari-
All SEM specimens were dehydrated in ascending grades sons. Statistical analyses were performed with the Sigma
of tert-butyl alcohol (50% for 20 min, 75% for 20 min, 95% Plot software system (v. 11.0, SPSS; Chicago, IL, USA).
for 20 min, and 100% for 2 h) and transferred from the final
100% bath to a critical-point dryer (Model ID-3, Elionix) for
30 min. Resin/enamel interface specimens were then sub- RESULTS
jected to argon-ion beam etching (EIS-200ER, Elionix) for 40 s
with the ion beam (accelerating voltage 1.0 kV, ion current Shear Bond Strength Tests
density 0.4 mA/cm2) directed perpendicular to the polished The results of the SBS test to enamel are shown in Table 3.
surfaces. Finally, all of the SEM specimens were coated in a Three-way ANOVA revealed that all the factors evaluated
vacuum evaporator (Quick Coater Type SC-701, Sanyu Denchi; (etching mode, application time, and adhesive) significantly
Tokyo, Japan) with a thin film of gold. Observation was car- influenced the SBS (p < 0.001, p = 0.031, and p < 0.001,
ried out in the SEM at an operating voltage of 10 kV. respectively). The three-way interaction between the factors
was significant (p < 0.001). Although the interaction between
Statistical Analysis application time and adhesive was not significant
Because of their homogeneity of variance (Bartlett’s test) and (p = 0.775), the other pairwise interactions were (p < 0.001).
normal distribution (Kolmogorov-Smirnov test), the data were For the self-etch mode, although there was no significant
subjected to ANOVA. A three-way ANOVA followed by Tukey’s difference in SBS among the adhesives in the PA group,
Honestly Significant Difference test was used for analysis of the shear bond strengths in the IA group showed a different
all numerical data (D = 0.05). To understand the relation- pattern. Regarding the etch-and-rinse mode, GP showed a

70 The Journal of Adhesive Dentistry

 Sai et al

Table 6 Influence of active application duration on total surface free energy

Baseline (4000 grit) Baseline (pre-etching)

60.0 (1.5)aB 60.0 (1.5)bB 77.7 (2.2)aA 77.7 (2.2)aA

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 50.6 (2.5)cAB 48.8 (2.5)bcB 53.0 (3.1)cA 52.5 (2.3)dA

SU 60.3 (2.7)aC 51.9 (3.4)bD 74.4 (2.9)aA 66.6 (4.8)cB

AU 55.8 (2.7)bB 47.1 (2.6)cC 62.7 (4.2)bA 50.7 (3.0)dC

CQ 47.6 (1.7)dB 45.9 (3.9)cB 54.8 (2.7)cA 48.7 (2.0)dB

BM 46.6 (1.8)dC 49.1 (1.8)bcC 60.5 (5.1)bB 72.4 (3.1)bA

N = 10, mean (SD) in mN•m-1. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital
letters in rows indicate no difference at the 5% significance level.

Table 7 Influence of application duration on dispersion force

Baseline (4000 grit) Baseline (pre-etching)

41.5 (0.2)aA 41.5 (0.2)aA 41.6 (2.2)aA 41.6 (0.2)aA

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 42.2 (1.2)aA 42.4 (0.8)aA 41.6 (1.0)aA 41.6 (0.8)aA

SU 42.5 (1.2)aA 41.6 (1.0)aA 41.7 (0.8)aA 41.6 (1.0)aA

AU 42.9 (0.9)aA 42.2 (1.0)aA 42.7 (0.9)aA 42.3 (1.2)aA

CQ 42.7 (0.8)aA 41.4 (1.0)aA 41.7 (0.9)aA 42.4 (1.0)aA

BM 42.7 (1.2)aA 42.2 (1.3)aA 42.8 (0.8)aA 42.1 (0.9)aA

N = 10, mean (SD) in mN•m-1. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital
letters in rows indicate no difference at the 5% significance level.

significantly lower SBS than did the other adhesives in the
IA group, which did not differ significantly from each other.
On the other hand, the SBS values in the PA group were
adhesive dependent. When comparing the different bonding
procedures for each adhesive, all the adhesives showed
significantly higher SBS in the etch-and-rinse mode than in
the self-etch mode, regardless of the application time.
However, the influence of application time on enamel SBS
was different in different etching modes. For the self-etch
mode, all tested materials had a lower SBS in the IA group
than in the PA group, and the difference was significant for
SU and AU. For the etch-and-rinse mode, no significant dif-
ferences in SBS were observed for any adhesives between
the IA and PA groups, nor was there any consistent trend.
Failure Mode Analysis of Debonded Specimens
The frequency of different failure modes after the SBS test is
shown in Table 4. Regardless of the etching and application
time, the predominant mode of failure for debonded speci-
mens was adhesive in the self-etch mode for all adhesives.
However, the frequency of mixed and cohesive failures in
enamel was higher in the etch-and-rinse mode with both ap-
plication times for all the adhesives, with the exception of GP.
Surface Roughness
The Ra values are shown in Table 5. The three-way ANOVA
revealed that pre-etching, application time, and adhesive type
significantly influenced Ra values (p < 0.001). The three-way
interaction between the factors was significant (p < 0.001),
as were all the pairwise interactions (p < 0.001).
All the adhesives showed significantly higher Ra values
in the etch-and-rinse mode than in the self-etch mode, re-
gardless of the application time. In self-etch mode, all the
adhesives showed significantly higher Ra values than the
initial baseline #4000-grit polished surface, and GP showed
significantly higher Ra values than the other adhesives, re-
gardless of the application time. When comparing the IA
and PA groups in the self-etch mode, all the adhesives

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Sai et al

Table 8 Influence of application duration on polar force

Baseline (4000 grit) Baseline (pre-etching)

3.0 (0.6)cB 3.0 (0.6)cB 9.6 (1.2)abA 9.6 (1.2)abA

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 6.6 (1.8)bB 6.3 (0.1)aB 10.3 (1.7)aA 10.9 (2.1)aA

SU 9.2 (1.6)aA 5.2 (1.5)abB 10.2 (1.4)aA 10.4 (1.5)aA

AU 5.6 (1.7)bA 2.6 (2.1)cB 4.3 (2.1)bAB 6.5 (1.9)cA

CQ 3.8 (0.5)cC 4.4 (1.5)bcC 10.3 (1.4)aA 6.0 (1.5)cB

BM 3.6 (0.7)cB 6.3 (1.4)aA 3.6 (0.9)bB 7.6 (2.1)bcA

N = 10, mean (SD) in mN•m-1. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital
letters in rows indicate no difference at the 5% significance level.

Table 9 Influence of application duration on hydrogen-bonding force

Baseline (4000 grit) Baseline (pre-etching)

15.5 (2.8)aB 15.5 (2.8)aB 26.5 (2.2)aA 26.5 (2.2)aA

Self-etch mode Etch-and-rinse mode

IA PA IA PA
GP 1.7 (0.6)dA 0.4 (0.1)cBC 0.8 (0.3)dB 0.1 (0.1)eC

SU 11.3 (2.1)bB 6.2 (1.3)bC 22.5 (2.5)bA 14.8 (2.6)cB

AU 8.0 (0.6)cB 5.6 (0.4)bB 15.7 (3.6)cA 11.9 (0.3)dB

CQ 1.1 (0.4)dB 0.1 (0.1)cC 2.8 (0.6)dA 0.3 (0.1)eC

BM 0.3 (0.1)eC 0.6 (0.1)cC 14.1 (2.7)cB 22.7 (2.2)bA

N = 10, mean (SD) in mN•m-1. Same superscript lowercase letters in columns indicate no difference at the 5% significance level. Same superscript capital
letters in rows indicate no difference at the 5% significance level.

showed significantly higher Ra values in the PA group than
in the IA group, with the exception of CQ. In the etch-and-
rinse mode, although AU and SU in the IA group showed no
significant differences in Ra values when compared to the
baseline pre-etching group, AU and SU showed significantly
lower Ra values in the PA group than in the baseline pre-
etching group and the IA group.
Surface Free Energy
The SFEs and their components are shown in Fig 1 and Ta-
bles 6–9. The three-way ANOVA revealed that all the factors
evaluated significantly influenced the JS values (p < 0.001).
The three-way interaction between the factors was signifi-
cant (p < 0.001), as were all the pairwise interactions
(etching mode vs adhesive p < 0.001, and application time
vs adhesive p < 0.001, respectively), with the exception of
etching mode and application time (p = 0.083).
Most adhesives showed significantly lower JS values in
the self-etch mode than the initial baseline (400-grit SiC).
Although GB, CQ, and BM did not show any significant differ-
ences between the IA and PA groups in the self-etch mode,
SU and AU showed significantly lower JS values in the PA
group than the IA group. Most adhesives showed significantly
lower JS values in the etch-and-rinse mode than the baseline
pre-etching values. For most adhesives, JS values in the etch-
and-rinse mode were higher than in the self-etch mode, re-
gardless of the application time. When comparing the appli-
cation time in the etch-and-rinse mode, only BM showed a
higher JS value in the PA group than in the IA group.
Regarding the dispersion force, all the groups showed a
similar dispersion force (JSd) of approximately 40 (mN • m-1),
and there were no significant differences between the bond-
ing procedure groups (Table 7). However, polar force (JSp)
and hydrogen-bonding force (JSh) were group dependent
(Tables 8 and 9). For JSp, baseline pre-etched specimens
showed a higher value than the initial baseline (400-grit SiC)
specimens, and most adhesives showed higher JSp values
in the etch-and-rinse mode than in the self-etch mode. When
comparing application time in self-etch mode, SU and AU
showed significantly lower JSp values in the PA group than

72 The Journal of Adhesive Dentistry

 Sai et al

Fig 2 Representative SEM images of a b

enamel surface treated with different bond-
ing procedures, 5000X magnification. a: GP
with IA in self-etch mode; b: GP with PA in
self-etch mode; c: GP with IA in etch-and-
rinse mode; d: GP with PA in etch-and-rinse
mode.

NU3912 5PL x5.000 NU3924 5PL x5.000

c d

NU3899 5PL x5.000 NU3927 5P L x5.000

Fig 3 Representative SEM images of a b

enamel surface treated with different bond-
ing procedures, 5000X magnification. a:
CQ with IA in self-etch mode; b: CQ with PA
in self-etch mode; c: CQ with IA in etch-and-
rinse mode; d: CQ with PA in etch-and-rinse
mode.

NU3951 5PL x5.000 NU3957 5PL x5.000

c d

NU3942 5PL x5.000 NU3969 5PL x5.000

in the IA group. Regarding the JSh values, baseline pre-
etched specimens showed a higher value than the initial
baseline (400-grit SiC) specimens, similar to the JSp val-
ues. All the adhesives showed significantly lower values in
the self-etch mode than the initial baseline values (400-
grit SiC). In addition, a similar trend was observed in the
etch-and-rinse mode, in that adhesive-treated specimens
had lower JSh values than the baseline pre-etching speci-
mens. Apart from BM, all the adhesives in the PA group
showed lower JSh values in the IA group, regardless of the
etching mode.
Interrelationships Between the Tested Parameters
The relationships between the parameters tested in this
study were measured using the Pearson product-moment
correlation coefficient. Strong positive correlations were ob-
served between SBS and Ra (r = 0.909, p = 0.008), while
weak correlations were observed between SBS and SFE
(r = 0.491, p = 0.028), Ra and SFE (r = 0.565, p = 0.009).
SEM Observations
Representative SEM images of treated enamel surfaces
from different bonding procedures are shown in Figs 2–4.
Apart from GP, all the universal adhesives had a similar

Vol 20, No 1, 2018 73

Sai et al

a b Fig 4 Representative SEM images of

enamel surface treated with different bonding
procedures, 5000X magnification. a: SU with
IA in self-etch mode; b; SU with PA in self-
etch mode; c: SU with IA in etch-and-rinse
mode; d: SU with PA in etch-and-rinse mode.

NU5902 5PL x5.000 NU3890 5PL x5.000

c d

NU3866 5PL x5.000 NU3881 5PL x5.000

a b Fig 5 Representative SEM micrographs of

the resin-enamel interfaces. Ad: adhesive,
En: enamel, RC: resin composite. The main
images are 5000X magnification. The
smaller white rectangles indicate the loca-
tion in the main image of the enlarged
area, at 20,000X, in the upper left corner.
Arrows indicate the smear layer. a: BM with
IA with self-etch mode; b: BM with PA with
self-etch mode; c: BM with IA with etch-and-
rinse mode; d: BM with PA with etch-and-
NU4185 5PL x5.000 NU3924 5PL x5.000
rinse mode.
c d

NU4217 5PL x5.000 NU4259 5PL x5.000

morphological appearance in the self-etch mode, that is,
the scratch marks remained and the standard etching pat-
tern was not observed regardless of application time
(Figs 3a, 3b, 4a, 4b). On the other hand, in SEM images of
GP over both application times in the self-etch mode, the
smear layer was completely dissolved and a shallow etch-
ing pattern was observed (Figs 2a, 2b). In the etch-and-
rinse mode, although all the tested adhesives showed a
similar morphological appearance in the IA group (Figs 2c,
3c, and 4c), morphological appearances in PA group were
adhesive dependent (Figs 2d, 3d, and 4d).
Representative SEM images of the resin/enamel inter-
face are shown in Figs 5–7. For all the tested adhesives in
both the IA and PA groups, the smear layer was completely
removed in etch-and-rinse mode. In the etch-and-rinse
mode, SU and AU showed more interpenetration of the resin
and enamel in the IA group than in the PA group in contrast
to GP, CQ, and BM. For both application times in the self-
etch mode, apart from GP, although a smear layer was ob-
served above the enamel surface, the state of the smear
layer was different between the IA and PA groups. That is,
more remnant smear layer was visible in the IA group than

74 The Journal of Adhesive Dentistry

 Sai et al

Fig 6 Representative SEM micrographs of a b

the resin-enamel interfaces. Ad: adhesive,
En: enamel, RC: resin composite. The main
images are 5000X magnification. The smaller
white rectangles indicate the location in the
main image of the enlarged area, at
20,000X, in the upper left corner. Arrows indi-
cate the smear layer. a: CQ with IA with self-
etch mode; b: CQ with PA with self-etch
mode; c: CQ with IA with etch-and-rinse mode;
d: CQ with PA with etch-and-rinse mode.
NU4149 5PL x5.000 NU4101 5P L x5.000

c d

NU4081 5PL x5.000 NU4165 5P L x5.000

Fig 7 Representative SEM micrographs of a b

the resin-enamel interfaces. Ad: adhesive,
En: enamel, RC: resin composite. The main
images are 5000X magnification. The
smaller white rectangles indicate the loca-
tion in the main image of the enlarged area,
at 20,000X, in the upper left corner. Arrows
indicate the smear layer. a: SU with IA with
self-etch mode; b: SU with PA with self-etch
mode; c: SU with IA with etch-and-rinse mode;
d: SU with PA with etch-and-rinse mode.
NU4372 5PL x5.000 NU4297 5P L x5.000

c d

NU4343 5PL x5.000 NU4321 5P L x5.000

in the PA group (Figs 5a, 6a, and 7a). The adhesive layer
thickness for all the tested adhesives was 7–10 μm, and
nanofillers were observed in the adhesive layer (Figs 5–7).
DISCUSSION
The optimal bonding procedure, including application meth-
ods and time, can differ completely from one adhesive or
clinical situation to another; therefore, the influence of ap-
plication time in different etching modes for universal adhe-
sives on enamel bond efficacy was investigated. The three-
way ANOVA results for the SBS test revealed that the
etching mode, application time, and adhesive type signifi-
cantly influenced the SBS. Therefore, the first null hypoth-
esis that application time would not affect the enamel SBS
irrespective of the etching mode was rejected. As expected,
SBS was higher in the etch-and-rinse mode than in the self-
etch mode, regardless of the adhesive type and application
time. However, the influence of application time on enamel
SBS was different in the two etching modes. In the self-etch
mode, all adhesives showed higher SBS in the PA group

Vol 20, No 1, 2018 75

Sai et al
than in the IA group. In particular, SU and AU showed sig-
nificantly higher values. On the other hand, SU and AU in
the etch-and-rinse mode showed lower SBS in the PA group
than in the IA group. These results suggested that the
enamel bonding performance of SU and AU was susceptible
to the influence of application time in different etching
modes. It can be speculated that the prolonged application
time of SU and AU in the PA group contributed to the in-
creased SBS in the self-etch mode. The manufacturers of
SU and AU recommend applying the adhesive with a rub-
bing motion for 20 s. The effect of a rubbing motion in in-
creasing enamel bond strength has been reported in previ-
ous studies,1,10,12,22 and Yoshihara et al27 demonstrated
that self-assembled nanolayering of calcium salt due to
chemical interaction was greater with a rubbing motion than
without a rubbing motion using a two-step self-etch adhe-
sive. On the other hand, the reason for the reduced SBS in
the PA group compared to the IA group for SU and AU in the
etch-and-rinse mode is that the force of the microbrush in
active motion collapses the spicular etching pattern with
increased application time.10 This might lead to a reduction
in micromechanical interlocking effects due to the collapse
of interspaces for resin monomer penetration.
Since strong positive correlations (r = 0.909, p < 0.001)
were observed between SBS and Ra values, micromechani-
cal interlocking is thought to be a very important factor for
generating adhesion to enamel. When comparing Ra values
between the self-etch and etch-and-rinse modes, the etch-
and-rinse mode showed values 5 to 7 times higher than the
self-etch mode regardless of the application time or adhe-
sive type. In the observations of fracture patterns, although
the predominant mode of failure was adhesive in the self-
etch mode, the frequency of mixed failure involving enamel
substrate and cohesive failure in enamel tended to in-
crease in the etch-and-rinse mode regardless of the applica-
tion time. Therefore, fracture analysis of debonded speci-
mens suggested that phosphoric acid pre-etching can
contribute to enamel adhesion by establishing microme-
chanical interlocking.
Previous studies have demonstrated the efficacy of phos-
phoric acid pre-etching for self-etch adhesives, including the
new category of universal adhesives.2,7,19,21 In contrast, a
study investigating the enamel bond durability of universal
adhesives in the self-etch mode under different aging condi-
tions, specifically 2-year water storage and thermocycling,
found no significant differences in SBS between baseline
groups and aged groups.18 Tsuchiya et al23 analyzed the
effect of functional monomers on enamel bond durability
using self-etch adhesives that differed only in the presence
or absence of the functional monomer 10-methacryloyl-
oxydecyl dihydrogen phosphate (MDP). Although no signifi-
cant difference was observed between the two adhesives in
initial bond strength when phosphoric acid pre-etching was
performed compared to bond strength after 1-year water
storage, the MDP-containing adhesive showed significantly
higher bond strength than did the the MDP-free adhesive.
Although mechanical interlocking on the enamel surface is
important, the formation of a strong chemical bond with the
76
enamel surface is also important.28 Hence, the application
time of universal adhesives may enhance the quality of
chemical bonding regardless of the etching mode.
In order to understand the state of chemical interactions
between universal adhesives and the enamel surface, the
SFE characteristic was determined. The three-way ANOVA of
JS results revealed that the etching mode, adhesive, and
application time significantly influenced the JS. Therefore,
the second null hypothesis that application time would not
affect the SFE irrespective of the etching method was re-
jected. Most tested adhesives had JS values in the self-etch
mode that were significantly lower than those of the initial
baseline group, and values in the etch-and-rinse mode that
were significantly lower than those of the pre-etched base-
line group, regardless of the application time. This phenom-
enon might be explained by the formation of a monomer-
calcium salt-layered structure on the HAp, and this chemical
interaction might occur very quickly, within a few seconds
after application of the adhesive.
In this study, the JS value was expressed as the sum of
three parameters: JSd, JSp, and JSh. Since the JSd did not
show any significant differences between the conditions,
the results for the other two parameters were strongly re-
lated to the changes in the JS value. JSp is thought to be
related to electric and metallic interactions in addition to
dipolar interactions, whereas JSh represents the water and
hydroxyl components of the substrate.24 In particular, JSh
parameters are helpful to identify whether the surface char-
acteristics lean toward hydrophilic or hydrophobic, since
substrates with higher JSh values tend to be soluble in
water, whereas substrates with lower JSh values tends to be
soluble in organic solvents. Looking at the influence of dif-
ferent bonding procedures on the JS of the tested adhe-
sives, SU and AU showed lower JS values in the PA group
than in the IA group, regardless of the etching mode. This
indicated that PA time and a rubbing motion might be help-
ful to induce chemical reactions.1,3,4,10,12,20,22
Increased chemical bonding intensity might be respon-
sible for the higher bond strength of SU and AU in the PA
group. GP and CQ also showed lower JS values in the PA
group than in the IA group, similar to SU and AU. Therefore,
although the chemical reaction might occur quickly within a
few seconds after the application of the GP and CQ adhe-
sives, the quantity and quality of chemical interaction might
be higher with a prolonged application time. On the other
hand, BM showed higher JS values in the PA group than in
the IA group, regardless of the etching mode. Further re-
search should be carried out to understand why BM be-
haved differently than the other adhesives.
The clinical indication from the present study is that the
reduced application time for universal adhesives might be
acceptable in the etch-and-rinse mode. For universal adhe-
sives that manufacturers recommend air blowing immedi-
ately after application, this procedure might be acceptable
in self-etch mode. However, when bonding to uncut enamel
surfaces, it is preferable to prolong adhesive application
time in self-etch mode or to use phosphoric acid pre-etch-
ing. Further research is needed to investigate the influence
The Journal of Adhesive Dentistry

of application time on the long-term stability of bonded res-
toration using universal adhesives.
CONCLUSION
The enamel SBS and Ra values of the tested universal ad-
hesives in the etch-and-rinse mode showed significantly
higher values than in the self-etch mode, regardless of the
application time. Although all the tested adhesives showed
increased SBS and Ra values with increased application
time in the self-etch mode, SU and AU showed decreased
SBS and Ra values with increased application time in the
etch-and-rinse mode. Regarding the SFE, all the tested uni-
versal adhesives showed decreased JS values with in-
creased application time in the self-etch mode, with the
exception of BM. However, JS values in the etch-and-rinse
mode were dependent on the adhesive type and application
time. The etching mode, application time, and type of adhe-
sive significantly influenced the SBS, Ra, and SFE values.
ACKNOWLEDGMENTS
This work was supported in part by Grants-in-Aid for Scientific Re-
search, No. 16K11565, 16K20465, 17K11716, and 17K17141 from
the Japan Society for the Promotion of Science. This project was also
supported in part by the Sato Fund and by a grant from the Dental Re-
search Center of the Nihon University School of Dentistry, Japan.
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Clinical relevance: In contrast to the etch-and-rinse mode,
care should be taken with the self-etch mode to ensure
that the clinical method employed to reduce adhesive ap-
plication time has no negative impacts on the enamel
bonding performance of some universal adhesives.
77