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Immediate and 6-month Bond Strengths of Different

Adhesives in the Oral Environment


Jamille Favarãoa / Maurício Matté Zaninib / Mário Alexandre Coelho Sinhoretic / Gabriel Flores Abunad /
Cláudio Girelli Júniore / Veridiana Camilottif / Marcelo Gianninig / Marcio José Mendonçah

Purpose: To evaluate the microtensile bond strength (μTBS) of three adhesives to dentin after 1 week and
6 months in an oral environment.
Materials and Methods: Class I cavities were prepared in the third molars of 30 patients and randomized into
3 groups according to the following adhesives: Scotchbond Multi-Purpose (SM), Clearfil Protect Bond (CF), and
Scotchbond Universal (UN). These molars were then subdivided into two groups according to the exposure time in
the oral environment: one week (1W) and 6 months (6M). After the exposure time, the teeth were extracted, cut
into beams, and submitted to the μTBS test. The data were analyzed using the Shapiro-Wilk test and two-way
ANOVA followed by Tukey’s post-hoc test with a significance level of 5%, and fracture modes were analyzed.
Results: The bond strengths in MPa (mean ± SD) were SM-1W: 39.5 ± 7.9; SM-6M: 29.7 ± 1.8; CF-1W:
30.5 ± 1.4; CF-6M: 28.6 ± 4.1; UN-1W: 30.6 ± 3.2; and UN-6M: 26.7 ± 2.0. The SM-1W group exhibited signifi-
cantly increased μTBS compared with the other groups. After 6 months in the oral environment, a significant re-
duction of μTBS was only observed for the SM group, whereas similar bond strengths were observed for the other
groups. SM-1W exhibited a predominance of mixed fractures, whereas the other groups showed a predominance
of adhesive fractures.
Conclusions: The adhesives which were applied in the self-etching mode maintained bond strength after six
months in the oral environment. A reduction of μTBS was only observed for the three-step etch-and-rinse adhesive.
Key words: dentin bonding agents, tensile strength, dentin, clinical study.

J Adhes Dent 2017; 19: 475–481. Submitted for publication: 04.08.17; accepted for publication: 02.12.17
doi: 10.3290/j.jad.a39594

T he adhesive strategies currently employed for dentin


bonding include etch-and-rinse or self-etch ap-
proaches.23 An initial etching step followed by a rinsing
Self-etching adhesives incorporate a dissolved smear
layer and demineralized dentin components. These adhe-
sives do not require a separate etching step because they
phase, a priming step and the application of hydrophobic contain acidic resin monomers that simultaneously “etch“
resin is necessary for three-step etch-and-rinse adhesives. and “prime“ the dental substrates.3 The process has been
Two-step etch-and-rinse adhesives combine the primer and further simplified by reducing the number of steps from the
hydrophobic resin into one application, and the mechanism initial two-step adhesive (an acidic primer followed by the
is principally based on the combined effect of hybridization application of a relatively hydrophobic bonding resin on top
and resin tag formation.22 of the primed surface) to a one-step adhesive, in which all

a PhD Student, Department of Restorative Dentistry, Dental Materials Division, f Adjunctive Professor, Department of Prosthodontics, University Estadual do
Piracicaba Dental School, University of Campinas, Piracicaba, São Paulo, Bra- Oeste do Paraná, UNIOESTE, Cascavel, Paraná, Brazil. Experimental design.
zil. Performed restorations, wrote the manuscript. g Professor, Department of Restorative Dentistry, Operative Dentistry Division,
b PhD Student, Department of Restorative Dentistry, Dental Materials Division, Piracicaba Dental School, University of Campinas, Piracicaba, São Paulo,
Piracicaba Dental School, University of Campinas, Piracicaba, São Paulo, Brazil. Brazil. Contributed substantially to the discussion.
Performed microtensile test, and statistical evaluation. h Adjunctive Professor, Department of Prosthodontics, University Estadual do
c Professor, Department of Restorative Dentistry, Dental Materials Division, Oeste do Paraná, UNIOESTE, Cascavel, Paraná, Brazil. Idea and hypothesis.
Piracicaba Dental School, University of Campinas, Piracicaba, São Paulo,
Brazil. Contributed substantially to the discussion and proofread manuscript.
d PhD Student, Department of Restorative Dentistry, Dental Materials Division,
Piracicaba Dental School, University of Campinas, Piracicaba, São Paulo,
Brazil. Performed MEV images.
Correspondence: Jamille Favarão, Rua Rui Barbosa, 319 / Centro, Vera Cruz
e Dentist, Department of Prosthodontics, University Estadual do Oeste do do Oeste, Paraná, Brazil 85845-000. Tel: +55-45-99-983-0623;
Paraná, UNIOESTE, Cascavel, Paraná, Brazil. Performed exodontic surgery. e-mail: jamillefavarao@hotmail.com

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Favarão et al

Assessed eligibility (Np = 162)

Excluded (Np = 126)


Did not meet the inclusion criteria (Np = 121)
Under 18 years (Np = 7)
Included third molars (Np = 36)
Third molar badly positioned (Np = 53)
Third molar caries (Np = 13)
Restored third molars (Np = 4)
Systematic diseases (Np = 7)
Pregnant woman (Np = 1)
Refused to participate (Np = 5)

Randomized (Np = 36; Nt = 36)

Allocated to extraction after Allocated to extraction after


1 week (Np = 17; Nt = 17) 6 months (Np = 19; Nt = 19)

Restored using Restored using Restored using Restored using Restored using Restored using
Scotchbond Clearfil Protect Scotchbond Scotchbond Clearfil Protect Scotchbond
Multi-Purpose Bond Universal Multi-Purpose Bond Universal
(Np = 5; Nt = 5) (Np = 6; Nt = 6) (Np = 6; Nt = 6) (Np = 6; Nt = 6) (Np = 7; Nt = 7) (Np = 6; Nt = 6)

Discontinued intervention
Discontinued intervention (Np = 4; Nt = 4)
(Np = 2; Nt = 2) Pregnant woman
Dropouts (Np = 2; Nt = 2) (Np = 1; Nt = 1)
Dropouts (Np = 3; Nt = 3)

Extraction Extraction Extraction Extraction Extraction Extraction


Scotchbond Clearfil Protect Scotchbond Scotchbond Clearfil Protect Scotchbond
Multi-Purpose Bond Universal Multi-Purpose Bond Universal
(Np = 5; Nt = 5) (Np = 5; Nt = 5) (Np = 5; Nt = 5) (Np = 5; Nt = 5) (Np = 5; Nt = 5) (Np = 5; Nt = 5)

Fig 1 Flow diagram. Np = number of patients; Nt = number of teeth.

components (acidic primer and bonding resin) are incorpo- the effect of a single variable if all of the other variables are
rated into a single solution.22 kept constant.13
The elimination of separate etching and rinsing steps Although laboratory research can predict the clinical per-
has simplified the bonding technique and increased the formance of a new adhesive to a certain extent, a clinical
popularity of these adhesives in daily practice; however, study is always desirable to confirm these results and deter-
manufacturers understand that professionals apply their mine the clinical bonding efficacy of an adhesive in general
own criteria to selecting an adhesive strategy based on the dental practice. Several clinical co-variables that are unique
numbers of steps. Thus, more versatile adhesives that in- to the oral environment and affect the clinical performance
clude etch-and-rinse (two-step) and self-etch (one- or two- of adhesives have been described, such as moisture, physi-
step) options have been released. These new materials are cal stresses, chewing habits, dietary components, and
called “universal” or “multimode” adhesives and can be changes in temperature and pH. These variables may act
applied either with the etch-and-rinse or the self-etch tech- simultaneously to accelerate degradation of the adhesive
nique, thus enabling the practitioner to select a specific bonds or result in catastrophic or even fatigue failures.19
adhesive protocol.24 A significant reduction in bond strength occurs after long
The ability of an adhesive to bond to dentin is commonly periods in aqueous environments because absorbed water
tested using in vitro bond strength tests. These laboratory affects the mechanical properties of the resin matrix mater-
tests are designed to closely simulate optimal clinical con- ial and metalloproteinase activities.3 Therefore, the pur-
ditions and are much less expensive than clinical trials be- pose of this study was to compare the bond strength of
cause that they do not require several years to elicit mean- three adhesives (a 3-step etch-and-rinse, a 2-step self-etch,
ingful outcomes. In addition, laboratory testing can evaluate and a universal adhesive applied in the self-etch mode) to

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Favarão et al

Table 1 Experimental groups

Adhesives Exposure time in oral environment Manufacturer and lot

Scotchbond Multi-Purpose (3-step etch-and-rinse) 1W, control 3M; St Paul, MN, USA.
Primer: N478117
6M Adhesive: N465871

Clearfil Protect Bond (2-step self-etch) 1W Kuraray Noritake; Tokyo, Japan.


Primer: 00115A
6M Adhesive: 00212A

Scotchbond Universal (universal, self-etch mode) 1W 3M


504834
6M

W: week; M: month.

dentin in restorations of class I cavities after 1-week and (Mepisv, Nova DFL; Rio de Janeiro, RJ, Brazil); the teeth
6-month service in the oral environment. The null hypothe- were then cleaned with pumice and water followed by rins-
sis was that long-term exposure to the oral environment ing and drying.
and differences in adhesive composition and application Class I cavities were prepared (4 mm in width x 5 mm in
approach do not affect the microtensile bond strength length x 3 mm in depth) with the cavosurface margin in
(μTBS) to dentin. enamel, flat bottom wall, and parallel surrounding walls.
The cavity was prepared first using a spherical diamond bur
(#1014, KG Sorensen; Cotia, SP, Brazil), followed by a cy-
MATERIALS AND METHODS lindrical diamond bur (#2094, KG Sorensen), and finished
with a superfine diamond bur (#1093FF, KG Sorensen). The
The experimental design followed the Consolidated Stan- burs were replaced after five preparations to maintain cut-
dards of Reporting Trials (CONSORT) statement.20 This was ting efficacy. Cavity depth was measured with a millimeter
a randomized, blind, prospective clinical trial. All partici- periodontal probe (Golgran; São Caetano do Sul, SP, Bra-
pants were informed about the nature and objectives of the zil). The teeth receiving the conventional etch-and-rinse ad-
study; however, they were not aware of the adhesive that hesive (Scotchbond Multi-Purpose) were conditioned with
would be used in the restoration to be evaluated. 37% phosphoric acid (Condac 37, FGM; Joinville, Brazil).
The local Ethics Committee on Investigations Involving Clearfil Protect Bond and Scothcbond Universal were
Human Subjects reviewed and approved the protocol and applied in the self-etch mode. All adhesives were applied
consent form for this study. Written informed consent was according to the manufacturer’s instructions (Table 2).
obtained from all participants prior to starting treatment. All photoactivation procedures were performed using an
Based on pre-established criteria, 30 volunteers were se- LED-curing unit at 1200 mW/cm2 (Bluephase G2, Ivoclar
lected (Fig 1). Vivadent; Schaan, Liechtenstein). Filtek Z350 composite
A total of 162 participants with at least one sound third shade A2 (3M) was applied in 2-mm increments and light
molar indicated for extraction were examined by a pre-cali- cured for 20 s. Then, the occlusal adjustment of the restor-
brated operator to determine whether they met the following ations was performed with a diamond bur (#1111FF, KG
inclusion and exclusion criteria (Fig 1): good general health, Sorensen) so that the tooth presented occlusal contact.
at least 18 years of age, not allergic to any component of The restorations were finished with Enhance (Dentsply;
the materials used. Moreover, the participant’s teeth had to Petrópolis, RJ, Brazil) and polished with diamond felt disks
have occlusal contact and a position that allowed for abso- (FGM) and Prisma Gloss paste (Dentsply).
lute isolation and extraction without odontosection. The restored teeth remained in the oral environment for
Thirty patients were selected, with one tooth each to be periods of one week (± 1 day) or 6 months (± 7 days). After
restored. The patients were randomly assigned to 3 groups these periods, the teeth were extracted by a single special-
according to the adhesive used: Scotchbond Multi-Purpose ist in maxillofacial surgery, individually stored in 0.5% chlo-
(SM) (3M; St Paul, MN, USA); Clearfil Protect Bond (CF) (Ku- ramine solution for 1 week under refrigeration at 4°C, and
raray Noritake; Tokyo, Japan); Scotchbond Universal (UN) stored in distilled water at 37°C for 24 h.8
(3M). Each group was divided into two subgroups with 5 Two-mm increments of composite were added to the oc-
teeth per group according to the exposure time in the oral clusal surface of the composite restorations to obtain sam-
environment, 1 week or 6 months (Table 1).2,8 ples with a suitable length so that they could be adapted to
The same calibrated operator restored all teeth. Radio- the testing machine.
graphs were obtained using the panoramic and interproxi- The teeth were then positioned in a diamond cutting ma-
mal techniques. Before placing the rubber-dam, the oper- chine (Isomet 1000, Buehler; Lake Bluff, IL, USA) and sec-
ator anesthetized the teeth with 3% mepivacaine solution tioned in the mesiodistal and buccolingual directions to

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Favarão et al

Table 2 Composition and application mode

Adhesives Composition Application mode


Scotchbond Multi-Purpose Primer: HEMA, polyalkenoic acid polymer, water 1. Acid etch for 15 s, rinse for 15 s. Blot excess
water using absorbent paper.
Adhesive: bis-GMA, HEMA, tertiary amines, photo- 2. Apply one coat of primer.
initiator 3. Gently blow air for 5 s at 10 cm to evaporate solvent.
4. Apply one coat of adhesive.
5. Light cure for 10 s.

Clearfil Protect Bond Primer: MDPB, MDP, HEMA, hydrophilic aliphatic 1. Dispense the necessary amount of primer into a
methacrylate, water, CQ, dyes, initiators, well of the mixing dish immediately before
accelerators application. Avoid exposing the material to
Adhesive: MDP, bis-GMA, HEMA, hydrophobic operating light or natural light. After 3 min, apply to
aliphatic methacrylate, sodium fluoride, colloidal the entire cavity wall. Leave it in place for 20 s.
silica, CQ, initiators, accelerators Gently blow air to evaporate the volatile ingredients.
2. Dispense the necessary amount of bond into a
well of the mixing dish immediately before
application. Avoid exposing the material to
operating light or natural light. After 3 min, apply to
the entire cavity wall. Create a uniform bond film
using a gentle blow air.
3. Light cure for 10 s.

Scotchbond Universal MDP, bis-GMA, HEMA, decamethylene DMA, ethanol, 1. Apply the adhesive for 20 s with vigorous agitation.
water, silane treated silica, 2-propenoic acid, 2. Gently air thin for 5 s.
2-methyl-, reaction products with 1,10-decanediol 3. Light cure for 10 s.
and phosphorous oxide, copolymer of acrylic and
itaconic acid, dimethylaminobenzoate(−4),
camphorquinone, (dimethylamino)ethyl
methacrylate, methyl ethyl ketone

Table 3 Mean values and standard deviation of experimental groups’ bond strength (MPa)

Adhesive Exposure time

1 week 6 months
Scotchbond Multi-Purpose 39.5 ± 7.9Aa (control) 29.7 ± 1.8Ba

Clearfil Protect Bond 30.5 ± 1.4Ab 28.6 ± 4.1Aa

Scotchbond Universal 30.6 ± 3.2Ab 26.7 ± 2.0Aa

Different upper case letters represent statistically significant differences in rows. Different lower case letters indicate statistically significant differences in columns.

obtain sticks with a 0.75 ± 0.1 mm2 cross-sectional area8 Representative fractured sticks from each group were
and the long axis perpendicular to the pulp wall. Seven to desiccated, mounted in aluminum stubs, and sputter
ten sticks per tooth were obtained, of which the central five coated with gold (Balzers SCD 050 Sputter Coater, Balzers
were used for mechanical tests to standardize the location Union; Balzers, Liechtenstein) to analyze the fracture pat-
of the sticks. terns via SEM (JSM 5600 LV, JEOL; Tokyo, Japan).
The cross-sectional area of the sticks was measured The data were subjected to the Shapiro-Wilk test, a two-
with a digital caliper to transform kgf to MPa. Then, the way ANOVA, and Tukey’s post-hoc test at a pre-set alpha of
specimens were attached to a microtensile device (0G01, 0.05 using Bioestat 5.1 software (Maua Institute; São
Geraldeli’s jig) with a cyanoacrylate adhesive (Henkel; Paulo, AM, Brazil).
Itapevi, SP, Brazil) and loaded to failure in tension using a
universal testing machine (Instron 4411; Canton, MA, USA)
at a crosshead speed of 1.0 mm/min2 until failure. RESULTS
Fractured specimens were examined with an optical mi-
croscope (Leica Microsystems; Wetzlar, Germany) at 40X The mean μTBS, including the standard deviation, are pre-
magnification by a single blinded and calibrated operator to sented in Table 3.
determine the failure mode. Failure modes were classified Two-way ANOVA revealed significant differences
as adhesive, mixed or cohesive. (p < 0.05) among the adhesives and exposure time factors;

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Favarão et al

with the increase of exposure time in the oral environment,


there was a reduction in the dentin bond strength for one of 100%
the adhesives. Tukey’s post-hoc test demonstrated that the
use of SM adhesive with one week of oral environment ex- 80%
posure yielded μTBS that were significantly higher than
those of the other adhesives, which did not differ signifi- 60%
cantly. However, a reduction in bond strength to dentin was
observed only for the SM adhesive after six months. 40%
Fracture analysis revealed a predominance of mixed fail-
ures for SM at 1 week, whereas the SM (6 months), CF and 20%
UN adhesives showed increased percentages of adhesive
failures (Fig 2). Cohesive failures within dentin or resin were 0%
not observed. Figure 3 depicts representative SEM images

1S (Control)

6M

1S

6M

1S

6M
of the failures for each group.

DISCUSSION Scotchbond Clearfil Protect Scotchbond


Multi-Purpose Bond Universal
In the oral environment, a number of factors acting simulta-
neously, including moisture, physical stress, chewing hab- Mixed
its, dietary components, as well as changes in temperature Adhesive
and pH, may accelerate the degradation of adhesive bonds
or result in catastrophic or even fatigue failures. Thus, once Fig 2 Fracture pattern analysis in %.
an adhesive performs well in vitro, a clinical trial is neces-
sary to evaluate its efficacy.18 the initial μTBS.10 Similar results were found by Hamouda
Therefore, the present study was conducted using differ- et al,9 who compared the in vitro bond strength of self-etch
ent exposure times in the oral environment. Restorations and etch-and-rinse adhesives after 24 h and found that the
with different adhesives were performed to better under- latter adhesive exhibited significantly higher bond strength
stand the behavior of these adhesives in clinical conditions. (38.3 MPa).
In this study, the 3-step etch-and-rinse adhesive Scotch- Despite obtaining the best results after 1 week in the
bond Multi-Purpose exhibited the highest bond strengths oral environment, the etch-and-rinse adhesive showed a re-
after 1 week in the oral environment (39.5 MPa). This find- duction in bond strength of 25% (29.7 MPa) after 6 months.
ing was related to the increased retentive area on the den- Similar results were obtained by Hashimoto et al,11 who
tin surface created by phosphoric acid, as well as the pres- evaluated primary molars restored using Scotchbond
ence of the resin bond which sealed dentin and produced Multi-Purpose in vivo and observed a reduction in bond

D D
A A

C
a b

C
Fig 3 SEM micrographs of debonded speci-
mens. Images a and b show a mixed failure A
for group SM-1S, with remnants of the ad- C
hesive (A) and composite (C) attached to A
dentin (D). Images c and d show an adhe-
sive failure for group UN-6M, without expo-
c d
sure of dentin surface.

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Favarão et al

strengths after 1, 2, and 3 years in the oral environment. Wagner et al25 also found similar results to those of this
The in vitro results of Bravis et al,4 who evaluated the bond study. They evaluated the in vitro bond strength of universal
strength of etch-and-rinse and self-etch adhesives after adhesives and verified that these materials maintained the
250,000 cycles with mechanical loading of 80 N also re- bond strength after thermocycling. Marchesi et al15 re-
vealed a statistically significant reduction in bond strength ported that although Scotchbond Universal showed a reduc-
for the etch-and-rinse adhesive, whereas the self-etch adhe- tion in adhesive bond strength after 6 months of storage in
sive demonstrated no difference in bond strength after me- artificial saliva, the values were maintained after one year.
chanical loading. However, Muñoz et al16 evaluated the immediate in vitro
The reduction in bond strength may well have been re- bond strength of different adhesives (etch-and-rinse, two-
lated to collagen exposed during etching which was not filled step self-etch, and universal) and found that universal adhe-
by the adhesive; thus, it was degraded by the dentin matrix sives showed lower bond strength when compared with the
metalloproteinases (MMPs). In demineralized dentin, organic two-step self-etch adhesives.
matrix exposure is noted and essentially represented by type The differences in the results observed in certain labora-
I collagen and proteoglycans that should be completely infil- tory studies may be related to the aging methods. For ex-
trated by adhesive to form the hybrid layer.1 However, a de- ample, in many in vitro studies, the sticks are aged in dis-
crease in the diffusion gradient of the resin monomers re- tilled water or artificial saliva,12,14,15 which directly exposes
sults in a demineralized collagen matrix layer that is not filled the interface to the hydrolytic action of the storage solution.
with monomers.3 Even without bacterial exposure, collagen In the present study, however, the composite-dentin inter-
may be degraded by metalloproteinases present in the den- face was surrounded by enamel and only indirectly exposed
tin matrix, because MMPs are activated by the low-pH phos- to the oral environment.
phoric acid and are responsible for the collagen fibril triple- A fractured dental substrate is indicative of the formation
helix breakdown and its subsequent degradation.6 of a thick hybrid layer5 and is reflected in the mixed failure
The universal adhesive Scotchbond Universal (applied in mode observed in this study for Scotchbond Multi-Purpose
the self-etch mode) presented μTBS similar to that of after 1 week in the oral environment. In contrast, the self-
Clearfil Protect Bond and did not show reductions in μTBS etch adhesives form a thin hybrid layer and a chemical
after 6 months in the oral environment. Clearfil Protect bond with dentin, so the fractures of the specimens tend to
Bond is derived from Clearfil SE Bond, which is considered occur at the adhesive-dentin interface.21
a reference for all self-etch adhesives.7,18 However, Clearfil Although the bond strength of the etch-and-rinse adhe-
Protect Bond contains MDPB monomer (12 methacryloyloxy- sive decreased, its bond strength still remained satisfac-
dodecyl-pyridinium bromide), an antibacterial agent that co- tory. Hence, it can still be indicated, since no clinical dam-
polymerizes with other monomers after curing, in addition to age to the restoration would be incurred after 6 months in
10-MDP monomer.17 the oral environment. However, this study cannot predict a
Clearfil Protect Bond and Scotchbond Universal have a discontinuous reduction of the bond strength. Therefore, it
pH of approximately 2, which leads to partial demineraliza- would be interesting to use adhesives that are stable over
tion of dentin and leaves a substantial amount of hydroxy- time, because this factor brings greater certainty to the clin-
apatite around the collagen fibrils. Self-etch adhesives at ician that a restoration will not present problems in the long
this pH are considered mild, and the maintenance of hy- term.
droxyapatite protects the collagen fibrils against hydrolytic
and enzymatic degradation.3
The similar results for these two materials may have CONCLUSIONS
resulted from the presence of 10-MDP (10-methacryloyl-
oxydecyl dihydrogen phosphate), which chemically bonds to Clearfil Protect Bond and Scotchbond Universal, which were
dentin. This chemical interaction is effective because of applied in the self-etching mode, maintained their bond
the formation of a nanolayer on the adhesive interface, strength after six months in the oral environment.
which improves the mechanical resistance of this region.
The interaction of 10-MDP with dentin occurs via ionic
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Vol 19, No 6, 2017 481


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