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RESEARCH AND EDUCATION

Bond strength of adhesive luting systems


to human dentin and their durability
Marius Maaßen,a Sebastian Wille, Dr,b and Matthias Kern, Prof Dr med dent Habilc

Autopolymerizing and dual- ABSTRACT


polymerizing resin systems
Statement of problem. The durability of adhesive bonding systems to dentin is of importance for
consist of a primer or an ad- restoration longevity; therefore, new adhesive systems should be tested in vitro with long-term
hesive for conditioning the artificial aging before clinical application.
dental hard tissues and an
Purpose. The purpose of this in vitro study was to investigate the bonding durability of 3
adhesive resin to bond the
dual-polymerizing resins and 1 autopolymerizing resin to human dentin with their specific
restoration to the tooth. self-etching primers or adhesives.
Dental adhesives can be
divided into adhesives with a Material and methods. Acrylic resin tubes filled with composite resin were bonded to human
dentin disks using either an autopolymerizing resin system (Panavia 21) or dual-polymerizing
separate etching step (etch and
resin systems (Panavia V5, RelyX Ultimate, and Variolink Esthetic DC) together with the
rinse) and self-etching primers system-specific primer or adhesive. Tensile bond strength was tested after 3 days of water
or adhesives (self-etch). Self- storage or after 150 days of water storage with 37 500 thermocycles (5  C to 55  C). The failure
etching primers or adhesives mode was evaluated by using a light microscope. In addition, representative specimens were
have become popular since examined by using a scanning electron microscope.
they were developed in the Results. After 3 days, the median tensile bond strengths ranged from 18.8 to 29.1 MPa. After
mid-1990s.1 because of their artificial aging for 150 days, the median tensile bond strengths ranged from 14.7 to 25.6 MPa.
simplified and less time- The dual-polymerizing resins showed significantly higher bond strength than the
consuming clinical applica- autopolymerizing resin (P.05). Artificial aging with thermocycling had no statistically significant
tion.2,3 They do not require a influence on tensile bond strength for the adhesive resin systems tested (P>.05). The failure
separate etching step with mode was mainly adhesive for the autopolymerizing resin, whereas it was mainly cohesive for
4-7 the dual-polymerizing resins.
rinsing as they contain
acidic monomers that condi- Conclusions. The 3 tested dual-polymerization resin systems provided durable bond strengths to
tion and prime the dentin and dentin which were higher than those of the autopolymerizing resin. (J Prosthet Dent 2019;-:---)
enamel simultaneously.
Monomers infiltrate the dentin and combine with the unlikely.11 Self-etching primers combine the etching step
collagen and the hydroxyapatite to produce a hybrid with priming and bonding4 in a single application pro-
8,9 10
layer. Nakabayashi et al demonstrated the impor- cedure.1,12,13 These systems and their simplified appli-
tance of the hybrid layer for adhesive bonding. cation have not been universally accepted as they allow
Self-etching primers or adhesives are less technique- dentinal fluids to cross polymerized resins.14 However,
sensitive than total phosphoric acid etching systems as they have been reported to be reliable under different
excessive etching, which might result in microleakage, is clinical conditions.15

This study was financially supported by Kuraray Noritake Dental Inc, Osaka, Japan.
a
Graduate student, Department of Prosthodontics, Propaedeutics and Dental Materials, School of Dentistry, Christian-Albrechts University, Kiel, Germany.
b
Head of Dental Materials Science, Department of Prosthodontics, Propaedeutics and Dental Materials, School of Dentistry, Christian-Albrechts University, Kiel, Germany.
c
Director of the Clinic, Department of Prosthodontics, Propaedeutics and Dental Materials, School of Dentistry, Christian-Albrechts University, Kiel, Germany.

THE JOURNAL OF PROSTHETIC DENTISTRY 1


2 Volume - Issue -

cleaned with a pumice-water mixture by using a


Clinical Implications brush with a handpiece for 10 seconds, and sprayed
Self-etching primers and adhesives with their with water-air from a dental unit. The dentin disks
were distributed into 4 groups of 16 disks with respect
respective dual-polymerizing resins show promising
to the adhesive system used.
bonding durability to dentin in comparison with
Acrylic resin tubes with an inner diameter of 3.3 mm
autopolymerizing resins. Artificial aging with
and a height of 15.0 mm were filled with autopolymerizing
thermocycling had no statistically significant
resin (CLEARFIL CORE New Bond; Kuraray Noritake
influence on tensile bond strength for the adhesive
Dental Inc). An autopolymerizing resin (Panavia 21;
resin systems tested. However, clinical studies are
Kuraray Noritake Dental Inc) with a self-etching and
recommended.
autopolymerizing primer (ED primer; Kuraray Noritake
Dental Inc) was used as the control. The dual-
polymerizing Panavia V5 with Tooth Primer (Kuraray
After tooth preparation, a smear layer consisting of
Noritake Dental Inc), dual-polymerizing RelyX Ultimate
dentin debris remains on the tooth surface.16 A signifi-
with Scotchbond Universal (3M ESPE), and dual-
cant difference between etch-and-rinse systems and self-
polymerizing Variolink Esthetic DC with Adhese Univer-
etching systems is the handling of this smear layer. With
sal (Ivoclar Vivadent AG) served as test groups for recently
self-etching primers or adhesives, the smear layer re-
introduced self-etching primers or adhesives in combi-
mains on the tooth surface and is incorporated, while,
nation with dual-polymerizing adhesive resins. The tested
with etch-and-rinse systems, it is removed.1,17,18
composite resins and their corresponding composition
Autopolymerizing and dual-polymerizing resins are
and group codes are summarized in Table 1.
used to cement dental restorations, including inlays,
Seven minutes after the start of mixing the composite
onlays, crowns, fixed partial dentures, posts and metal
resin, the tubes were bonded with their respective adhesive
cores, implant abutments, and superstructures. They are
resins to the dentin specimens by using an alignment
compatible with many materials (metal, glass-ceramic,
apparatus with a load of 7.4 N. This bonding method has
lithium disilicate glass-ceramic, zirconia ceramic, and
been previously described in detail.26 Excess resin was
composite resin restorations). Autopolymerizing resins
removed from the bonded margin by using cotton pellets,
are polymerized chemically by an amine or peroxide
and a gel was then applied to prevent an oxygen-inhibited
system. Dual-polymerizing resins offer the beneficial
layer (Oxyguard II; Kuraray Noritake Dental Inc, for Pana-
option of additional light-activated polymerization by
via 21 and Panavia V5, and Liquid Strip; Ivoclar Vivadent
using photoinitiators such as the camphorquinone and
AG, for RelyX Ultimate and Variolink Esthetic DC).
amine systems.4,18-20
All specimens were then placed in an incubator at 37
The purpose of this in vitro study was to investigate 
C for 10 minutes. For polymerization of the dual-
the bonding capacity of 3 dual-polymerizing and 1
polymerizing systems, an LED polymerization lamp
autopolymerizing resin to human dentin when used with
(Radii-cal; SDI Limited) with a light power of 1200 mW/
their specific self-etching primer or adhesive systems.
cm2 at a wavelength of 440 nm to 480 nm was used.
Additionally, the bonding durability after artificial aging
Each bonding group was then randomly divided into
by long-term water storage and thermocycling was
2 subgroups (n=8) with respect to the storing conditions
evaluated.21,22 The null hypotheses were that the tensile
by drawing them blindly out of the group container
bond strengths of the adhesive systems to human dentin
(similar to drawing lottery tickets). One subgroup was
would be similar and that thermocycling would not affect
stored in water at 37  C for 3 days with no thermocycling,
the durability of the bond.
and the other was stored alternately in water at 37  C for
150 days with 37 500 thermocycles from 5  C to 55  C. A
MATERIAL AND METHODS
cycle consisted of 2 temperature-change loads. The dwell
Sixty-four caries-free extracted human third molars time in each bath was 30 seconds.27-29 After the different
were cleaned of periodontal tissue and stored in a 0.1% storage conditions, the tensile bond strength was eval-
thymol solution at 4  C. The teeth were processed uated at a cross-head speed of 2 mm/min in a universal
within 2 weeks after extraction. Dentin disks with a testing machine (Zwick Z010/TN2A; ZwickRoell GmbH
thickness of 3.5 mm were prepared by cutting buccal or & Co KG) by using a special test configuration, which
lingual dentin perpendicular to the tooth axis by using provided a moment-free axial force application. A collet
a slow-speed diamond saw (IsoMet; Buehler) under held the tube while an alignment jig allowed self-
water cooling. The specimens were embedded in an centering of the specimen.26
autopolymerizing resin (Luxatemp; DMG-Dental) in a Statistical software (IBM SPSS for Windows, v20.0;
brass ring. The specimens were wet polished with 600- IBM Corp) was used for the statistical analysis. The
grit SiC paper, stored in distilled water at 4  C,15,23-25 Shapiro-Wilk test revealed that the data of some groups

THE JOURNAL OF PROSTHETIC DENTISTRY Maaßen et al


- 2019 3

Table 1. List of bonding systems, manufacturer, and composition of cement and primer
Polymerization System Primer Adhesive
Mode (Group Code) Manufacturer Cement Composition Composition Composition
Autopolymerizing Panavia 21 Kuraray Base paste: Hydrophobic aromatic dimethacrylate, hydrophobic Liquid A: HEMA,
(P21) Noritake Dental aliphatic methacrylate, hydrophilic aliphatic dimethacrylate, MDP, 5-NMSA,
Inc silanated titanium oxide, silanated barium glass filler, catalysts, water, accelerators
accelerators, pigments Liquid B: 5-NMSA,
Catalyst paste: MDP, hydrophobic aromatic dimethacrylate, water, catalysts,
hydrophobic aliphatic methacrylate, silanated silica filler, colloidal accelerators
silica, catalysts
Dual-polymerizing Panavia V5 Kuraray Bis-GMA, TEGDMA, silanated barium glass filler, silanated Tooth primer:
(PV5) Noritake Dental fluoroaluminosilicate glass filler, colloidal silica, surface-treated HEMA, MDP,
Inc aluminum oxide filler, hydrophobic aromatic dimethacrylate, hydrophilic aliphatic
hydrophilic aliphatic dimethacrylate, CQ, initiators, accelerators, dimethacrylate,
pigments accelerators, water
Dual-polymerizing RelyX Ulitmate 3M Deutschland Base paste: glass powder surface modified with 2-propenoic acid, Scotchbond
(RXU) GmbH 2 methyl-, 3-(trimethoxysilyl)propyl esters and phenyltrimethoxy Universal: MDP,
silane, bulk material, 2-propenoic acid, 2-methyl-, 1,10 -[1- dimethacrylate
(hydroxymethyl)-1,2-ethanediyl] ester, reaction products with 2- resins, HEMA, CQ,
hydroxy-1,3-propanediyl dimethacrylate and phosphorus oxide, filler, ethanol, water,
TEGDMA, silane-treated silica oxide glass chemicals (nonfibrous), initiators, silane
sodium persulfate, tert-butyl peroxy-3,5,5 trimethylhexanoate,
acetic acid, copper(2+) salt, monohydrate
Catalyst paste: glass powder, surface modified with 2-propenoic
acid, 2 methyl-, 3-(trimethoxysilyl) propyl ester, bulk material,
substituted dimethacrylate, 2,4,6(1h,3h,5h)-pyrimidinetrione, 5-
phenyl-1-(phenylmethyl)-, calcium salt (2:1), 1,12-dodecane
dimethacrylate, silane-treated silicia, sodium P-toluenesulfinate,
p-2-propenoic acid, 2-methyl-, [(3-methoxypropyl) imino] di-2,1-
ethanediyl ester, calcium hydroxide, 2-propenoic acid, 2-methyl-,
2-[(2-hydroxyethyl) (3-methoxypropyl)amino]ethyl ester
Dual-polymerizing Variolink Ivoclar Vivadent Base paste: ytterbium trifluoride, UDMA, 1,10-decandiol Adhese Universal:
Esthetic DC AG dimethacrylate, acetyl-2-thiourea HEMA, Bis-GMA,
(VE) Catalyst paste: ytterbium trifluoride, UDMA, 1,10-decandiol ethanol, 1,10-
dimethacrylate, CHUP decandiol
dimethacrylate,
MDP, CQ,
dimethylaminoethyl
methacrylate

Bis-GMA, Bisphenol A diglycidylmethacrylate; CQ, dl-camphorquinone or campherquinone; CUHP, a,a-dimethylbenzyl hydroperoxide; HEMA, 2-hydroxyethylmethacrylate;
MDP, 10-methacryloyloxydecyl dihydrogen phosphate; 5-NMSA, N-methacryloyl-5-aminosalicylic acid; TEGDMA, triethylene glycol dimethacrylate; UDMA, urethane dimethacrylate.

were not normally distributed. Therefore, the data were The fracture modes of the 4 adhesive resin systems as
statistically evaluated with the Kruskal-Wallis test fol- a percentage of the bonding area are summarized in
lowed by a pairwise Mann-Whitney comparison (a=.05), Figure 1. The failure mode was mainly adhesive for the
and a Bonferroni-Holm correction for multiple compari- autopolymerizing resin, while it was mainly cohesive for
sons was conducted. the dual-polymerizing resins. In addition, no cohesive
The fractured interfaces of all specimens were examined failures in the dentin substrate were found in the auto-
visually by using a light microscope (Wild Makroskop polymerizing resin group. The other groups showed a
M420; Leica) at ×30 magnification to calculate the fractured limited number of cohesive failures in the dentin.
interfaces of the debonded specimens and to determine Representative SEM micrographs of the fracture in-
failure modes (adhesive, cohesive in dentin, or cohesive in terfaces are shown in Figures 2, 3.
resin).26 In addition, representative specimens were air-
dried for 24 hours and examined under a scanning electron DISCUSSION
microscope (SEM) operating with an acceleration voltage of
The bond strengths of the control autopolymerizing resin
15 kV (Philips XL 30 CP; Philips) after sputtering a gold
(Panavia 21) (14.7 to 18.8 MPa) are similar to those of
alloy conductive layer of approximately 15 nm.27,28,30
previous studies that reported a bond strength of 13.8 to
17.1 MPa.31-33 However, the dual-polymerizing resins
RESULTS
with their self-etching primers or adhesives showed
The tensile bond strengths of all groups and their sta- significantly higher bond strengths (23.8 to 29.1 MPa),
tistical analysis are presented in Table 2. The dual- consistent with the results of previous studies.19,24,34,35
polymerizing resins showed statistically, significantly, Based on the results of other studies and within the limi-
higher bond strengths than the control autopolymerizing tations of this study, the dual-polymerizing resins appear
resin (P.05). Artificial aging with thermocycling had no to be better than the control autopolymerizing resin.
statistically significant influence on tensile bond strength The null hypothesis that the adhesive systems do not
for the adhesive resins tested (P>.05). provide different tensile bond strengths to human dentin

Maaßen et al THE JOURNAL OF PROSTHETIC DENTISTRY


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Table 2. Medians and means ±standard deviation of tensile bond strength (MPa) of all subgroups (n=8)
3d 150 d
Groups Adhesives Primer Median Mean ±SD Median Mean ±SD
P21 Panavia 21 ED Primer 18.8Ba 19.2 ±2.7 14.7Ba 15.4 ±2.5
PV5 Panavia V5 Tooth Primer 26.5Aa 27.6 ±5.0 23.8Aa 25.7 ±4.2
VE Variolink Esthetic Adhese Universal 27.6Aa 28.1 ±3.5 24.3Aa 23.7 ±2.5
RXU RelyX Ultimate Scotchbond Universal 29.1Aa 28.9 ±3.5 25.6Aa 25.5 ±2.7

SD, standard deviation. Statistically different means (P.05) indicated by different superscript uppercase letters within column (same kind of storage conditions). Same subscript lowercase
letters indicate no statistically significant difference within row (same primer or adhesive system).

100% 0 0 3
11 9
90% 17
26 23
25
80% 20
20
70% 39
Bonding Area (%)

60% 80 82 34
35
50%

40%
72 71
30% 63
50
20% 39 43

10% 20 18

0%
P21-3d P21-150d PV5-3d PV5-150d RXU-3d RXU-150d VE-3d VE-150d
Test Groups After 3 and 150 Days' Storage Time

Cohesive failure in resin Adhesive failure to dentin Cohesive failure in dentin

Figure 1. Graphical presentation of proportional prevalence of fracture modes of debonded dentin surfaces of all subgroups in percent.

was rejected as the bond strength of the autopolyme- Panavia V5 is not polymerized by light and therefore con-
rizing resin was significantly lower than that of the dual- tains no photoinitiator. Therefore, the presence of a pho-
polymerizing resins. The observed increased adhesive toinitiator does not appear to affect bond strength
failure mode of the autopolymerizing resin is consistent compared with the other dual-polymerizing primers.
with its lower bond strength compared with the dual- Further differences exist between the exposure times of the
polymerizing resins. In addition, the increasing number auto- and dual-polymerizing resin primers used. All
of cohesive failures with increased tensile strength is primers or adhesives of the dual-polymerizing resins
consistent with the observed failure types. moisten the dentin for 20 seconds, while the manufacturer
One reason for the different observed bond strength of the primer of the autopolymerizing resin recommends a
could be the composition of primer and adhesive resin. reaction of 60 seconds with the dentin.
The properties of self-etching primers are determined by Adequate demineralization of the hard tissue requires
components such as acidic monomers.6 These acidic a sufficiently low pH value in the self-etching primer or
monomers have a hydrophilic group that demineralizes adhesive. The primer of the autopolymerizing resin in
and forms a chemical bond to calcium and hydroxyapa- this study had a pH value of 3.0, while the pH values of
tite. In this study, different self-etching primers with the primers or adhesives of the dual-polymerizing resins
different compositions were tested. One commonality of were between 2.0 (PV5) and 2.7 (VE and RXU). The pH
all primers is the use of the acidic monomer 10- values of the primers correspond to the classification of
methacryloyloxydecyl dihydrogen phosphate (10-MDP) Van Meerbeek et al,21 mild (pHz2) and ultra-mild
and 2-2-hydroxyethylmethacrylate (HEMA). However, (pH2.5). Mild self-etching primers partially remove
the auto- and dual-polymerizing resins have different the smear layer, forming a thin hybrid layer. The dis-
primers or adhesives with camphorquinone as a photo- solved hydroxyapatite can then chemically bond with
initiator to light-polymerize the primer. Tooth primer of the functional monomers.4,7 Ultra-mild self-etching primers

THE JOURNAL OF PROSTHETIC DENTISTRY Maaßen et al


- 2019 5

Figure 2. SEM pictures from P21 after 150 days with low magnification (A, ×500) and higher magnification (B, ×1000) exhibit grooves from grit paper
grinding and shows hybrid layer remnants and dentinal tubes, which indicates adhesive failure.

Figure 3. SEM pictures from RXU after 150 days with low magnification (A, ×500) and higher magnification (B, ×1000) show composite resin remnants
and no dentinal tubes, which indicates cohesive failure in composite resin.

only expose superficial dentin, forming a nanometer- which prevent copolymerization.2,3,12,23 This could lead to a
thick interaction zone.4 Although the hybrid layer may lower bond strength to dentin compared with the faster
be important, its thickness and the associated relation to copolymerization of the dual-polymerizing resins when
tensile bond strength is still unclear.8,9 Therefore, the used with light-activated polymerization. Tagami et al24 and
mild pH value of the primer of the autopolymerizing Luhrs et al20 reported that faster polymerization had a
resin alone cannot be responsible for the lower observed positive effect on the bond strength when bonding to
bond strength. dentin with dual-polymerizing resins, as water droplets
In the past, single-bottle adhesives and auto- or dual- were prevented or at least reduced.
polymerizing composite resins have been reported to The null hypothesis that thermocycling does not affect
address issues of incompatibility.12,36 The acidic monomers the durability of the bond was confirmed because the
of the primer extract important amines from the redox thermocycling did not statistically significantly affect the
initiator system of the adhesive.12,36 These tertiary amines tensile bond strength to dentin. All the adhesive luting
are of importance for polymerizing with the redox initiator resin systems tested appear to have a good resistance
system. A decrease of amines leads to reduced polymeri- against hydrolysis and thermocycling during the tested
zation at the bonding interface, which might have led to time interval. The bonding interface must be resistant to
reduced bond strength with the autopolymerizing resin.12,36 the influences of the oral environment to be clinically
The lower bond strength of the autopolymerizing resin successful. Adequate artificial aging should provide com-
might be explained by its slow polymerization reaction, plete water saturation to the bonded interfaces over
causing water diffusion from the dentin across the hybrid months.37-40 Thermocycling with prolonged water storage
layer to the resin cement interface to form water droplets, is a common method of imitating thermal stress and water

Maaßen et al THE JOURNAL OF PROSTHETIC DENTISTRY


6 Volume - Issue -

absorption at the bonding interface in an attempt to 7. Yoshida Y, Nagakane K, Fukuda R, Nakayama Y, Okazaki M, Shintani H,
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Mde L, et al. Effect of smear layer thickness and acidity of self-etching so-
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12. Sanares AM, Itthagarun A, King NM, Tay FR, Pashley DH. Adverse surface
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42. Watanabe EK, Yatani H, Yamashita A, Ishikawa K, Suzuki K. Effects of Copyright © 2019 by the Editorial Council for The Journal of Prosthetic Dentistry.
thermocycling on the tensile bond strength between resin cement and https://doi.org/10.1016/j.prosdent.2019.07.012

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