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dental

materials
Dental Materials 18 (2002) 227±238
www.elsevier.com/locate/dental

The use of ¯owable composites as ®lled adhesives


Roland Frankenberger a,*, Manuela Lopes b, Jorge PerdigaÄo c, Wallace W. Ambrose d,
Bruno T. Rosa e
a
Policlinic for Operative Dentistry and Periodontology, University of Erlangen-Nuremberg, Glueckstrasse 11, D-91054 Erlangen, Germany
b
Minnesota Dental Research Center for Biomaterials and Biomechanics, University of Minnesota, 16-212 Moos Tower B 515 Delaware St SE, Minneapolis,
MN 55455, USA
c
Division of Operative Dentistry, Department of Restorative Sciences, University of Minnesota, 8-450 Moos Tower B 515 Delaware St SE, Minneapolis,
MN 55455, USA
d
School of Dentistry, Dental Research Center, University of North Carolina at Chapel Hill CB no. 7455, Chapel Hill, NC 27599-74550, USA
e
Private practice, Londrina, PR, Brazil
Received 17 October 2000; received in revised form 23 March 2001; accepted 9 April 2001

Abstract
Objective: The effect of ®lled adhesives on bonding resin composites to dentin has not been fully understood. Due to their ®ller content,
®lled adhesives may act as stress breakers. The aim of this in vitro study was to evaluate the use of ¯owable composites of different viscosities
on bonding to enamel and dentin without the use of an intermediate bonding resin.
Materials and methods: Enamel and dentin bond strengths of OptiBond FL, Syntac Classic, and EBS Multi combined either with their
proprietary bonding agent or a ¯owable resin composite (Ultraseal XT Plus or Revolution) were measured. The tests were carried out with a
microtensile device at a crosshead speed of 1 mm/min after 24 h of storage at 378C in water. Mean bond strengths were analyzed using the
Wilcoxon test and multiple comparisons according to the Mann-Whitney U-test. The micro-morphology of corresponding resin±dentin
interfaces of the same teeth were analyzed using SEM and TEM.
Results: The control groups with adhesive systems used as per manufacturers' protocol showed bond strengths of 38.9±41.1 MPa to
enamel and 28.8±33.4 MPa to dentin. With respect to bond strength to etched enamel, only Ultraseal XT Plus as bonding resin reached the
level of the control groups. When used as bonding agents on dentin, both ¯owable composites produced lower microtensile bond strengths to
etched and primed dentin than did the control groups. Micro-morphological analysis using SEM and TEM resulted in hybrid layer formation
for both control and experimental groups. However, many areas of the resin±dentin interface showed insuf®cient penetration of the ¯owable
composites at the top of the hybrid layer as well as numerous tubules obstructed by ®ller particles.
Conclusions: The ¯owable composites tested in this study should not be used to replace bonding agents. Flowable composites of thinner
viscosity, such as Ultraseal XT Plus, may bond to enamel adequately without the requirement of an intermediate bonding resin. q 2002
Academy of Dental Materials. Published by Elsevier Science Ltd. All rights reserved.
Keywords: Enamel bonding; Dentin bonding; Hybrid layer; Resin composites; Flowable composites; Filled adhesives

1. Introduction materials is fundamentally dependent on effective and


durable adhesion to enamel and dentin [6±8].
The increasing attractiveness of tooth-colored restora- Bonding to enamel is now accepted as clinically reliable,
tions has promoted research in this particular area of because acidic etchants, such as 30±40% phosphoric acid, are
operative dentistry during the last few years [1±3]. capable of creating microporosities on the enamel surface
For Class II restorations, resin-based restorative materials which enable the penetration of polymerizable monomers
are now being used instead of amalgam [4,5]. Due to the to provide micromechanical retention [9,10]. However,
characteristic polymerization shrinkage of resin-based dentin still remains an unpredictable substrate for adhesion.
composites, clinical success with composite restorative The wet tubular microstructure, combined with the high
organic content, is responsible for bonding to dentin being
far more dif®cult to perform [11±14]. Although different
* Corresponding author. Tel.: 149-9131-853669; fax: 149-9131-
approaches of surface pre-treatment are available, acid-
853603. etching and subsequent penetration of reactive primer
E-mail address: frankbg@dent.uni-erlangen.de (R. Frankenberger). molecules into the decalci®ed dentin surface is the most
0109-5641/02/$22.00 + 0.00 q 2002 Academy of Dental Materials. Published by Elsevier Science Ltd. All rights reserved.
PII: S0109-564 1(01)00040-9
228 R. Frankenberger et al. / Dental Materials 18 (2002) 227±238

recommended [2,14,15]. While modern one-bottle adhesives (SEM) and transmission electron microscopy (TEM)
combine primer and bonding resin in one solution, conven- evaluation.
tional two-bottle systems rely on a low-viscosity primer
acting exclusively for penetration and impregnation of the
collagen network exposed by acid etching [13,16,17]. High 2. Materials and methods
vapor-pressure solvents, like acetone or ethanol, are
commonly used to facilitate the penetration and carry the 2.1. Specimen preparation and microtensile testing
monomers into a direct contact with collagen ®bers [12,17±
19]. The primer is followed by a hydrophobic bonding resin A total of thirty six caries-free human third molars were
designed for ®lling the inter®brillar spaces as a backbone and used in this investigation. The teeth were stored in 0.1%
mechanically stabilizing the established interface generating thymol solution at ambient temperature for less than 4
a mixed zone of resin-entangled collagen ®brils, the hybrid weeks after extraction and were consecutively debrided
layer [20]. The use of these hybridizing adhesive systems has and examined to ensure that they were free of defects. For
been reported to produce high bond strengths, primarily when bond strength testing, the occlusal enamel was removed and
the dentin was left moist instead of being dried after etching 700±900 mm thick enamel±dentin disks were cut from the
and rinsing [6,12,18]. mid-coronal level of the tooth, perpendicular to the tooth
A modi®cation was introduced when ®lled bonding axis by slow-speed diamond-saw sectioning (Isomet,
resins, such as OptiBond FL (Kerr, Orange, CA, USA) Buehler, Lake Bluff, IL, USA) under continuous water cool-
and Permaquik (Ultradent Products, Inc., Salt Lake City, ing. A standardized smear layer was created in both corre-
UT, USA) were marketed [21,22]. After air thinning, the sponding surfaces by wet-sanding with 600-grit sandpaper
high viscosity of these adhesives results in thicker layers at for 60 s [17]. Eighteen teeth were randomly assigned to
both the cavity ¯oor and margin [6]. It has been repeatedly three dentin adhesives. Further, the teeth were subdivided
reported to be promising regarding marginal and internal into three groups with a ¯uid resin and two ¯owable resin
seal of resin composite restorations [23±26]. composites acting as bonding agent. Both surfaces were
This phenomenon characterized by a thicker adhesive treated with the adhesive systems (Table 1) OptiBond FL
layer between restorative material and tooth substrates (Kerr), Syntac Classic (Vivadent, Schaan, Principality of
was described as elastic cavity wall concept [26]. Using Liechtenstein), and EBS Multi (ESPE, Seefeld, Germany)
un®lled adhesives, extensive air thinning due to different according to the manufacturer's instructions except for
cavity geometries might result in thin layers which could Syntac classic which was applied upon etching dentin for
not be polymerized due to the polymerization inhibition by 15 s like alternatively recommended in the manufacturer's
oxygen [2,12]. Thicker layers of un®lled resins may there- protocol. The experimental groups were treated with the
fore be as advantageous for marginal adaptation as the primers like in the control groups but afterwards bonded
application of ®lled adhesives, but it cannot be recom- with the ¯owable resin composites Ultraseal XT Plus (Ultra-
mended clinically, because these materials usually provide dent Products, Inc., Salt Lake City, UT, USA) and Revolu-
no radiopacity [27]. Therefore, this modi®ed use could tion (Kerr, Orange, CA, USA) replacing the manufacturers'
mislead clinicians to interprete the adhesive radiotran- bonding resins and scrubbed continuously for 15 s onto the
sparency as gap formation or recurrent caries at the margin primed surface. The ¯owable composites acting as bonding
of the restoration [27]. agent were thinned with a brush but not air-thinned and
Flowable resin composites have been reported to adapt consecutively light-cured for 40 s. The crowns of the ¯at-
well to the cavity wall [5]. This optimal adaptation may tened teeth were then reconstructed with four 1 mm-layers
result in an improvement of the adhesive performance of of a mini®lled hybrid resin composite (Tetric Ceram,
resin composites [5,28,29]. Unterbrink and Liebenberg Vivadent) each layer being light-cured for 40 s with an
suggested using a ¯owable resin composite as bonding Elipar Highlight curing unit (without softstart). The intens-
agent to solve this problem by forming a strong and radio- ity of the light was checked periodically with a radiometer
paque material at the resin±dentin interface [30,31]. (Demetron/Kerr, Danbury, CT, USA) to ensure that an
Due to the fact that ®lled adhesives and ¯owable intensity 400 mW/cm 2 was exceeded. The disks made for
composites appear to have similar viscosities, this tech- micromorphological investigations were pretreated simul-
nique may have a strong impact for the restoration of taneously and covered with resin composite in one layer
carious lesions with direct resin composites. Nevertheless, of 1 mm thickness, then cut in half and stored in distilled
the effect of ¯owable composites on bond strengths and water for making the SEM and TEM specimens (Fig. 1).
interfacial micro-morphology has not been fully studied. The m-TBS specimens were stored in distilled water for
Therefore, the null hypothesis to be tested in this project 24 h at 378C and then sectioned. The peripheral areas of the
was that ¯owable composites would be as effective as tooth were removed resulting in a 5 £ 5 mm square central
un®lled bonding resins when used as part of a bonding part. The remaining specimen was sectioned into ®ve slices,
system, by using a microtensile bond strength test (m- which were sectioned again to receive 25 resin±dentin
TBS) combined with scanning electron microscopy beams. The saw was adjusted to steps of 1 mm, due to the
R. Frankenberger et al. / Dental Materials 18 (2002) 227±238 229

Table 1
Investigated adhesive systems, ¯owable resin composites replacing the bonding resins, and manufacturers

Adhesive Etchant Primer Bonding resin Manufacturer


system (code)

OptiBond FL Kerr Etchant OptiBond Primer OptiBond Adhesive Kerr, Orange,


CA, USA
37.5% phosphoric acid HEMA, GPDM, MMEP, ethanol, Bis-GMA, HEMA, GPDM, barium-
water, initiators aluminum borosilicate glass, disodium
hexa¯uorosilicate, fumed silica
(total ˆ 48% ®ller)
Ultraseal XT Plus (Ultradent)
Bis-GMA, TEGDMA, 53% ®ller
Revolution (Kerr)
Bis-GMA, TEGDMA, 53% ®ller
Syntac classic Total Etch Syntac classic primer Heliobond Vivadent, Schaan,
Liechtenstein
36% phosphoric acid Maleic acid, TEGDMA, water, acetone Bis-GMA, TEGDMA, UDMA
Syntac classic adhesive Ultraseal XT Plus
(2nd primer) Revolution
PEGDMA, glutaraldehyde, water
EBS Multi MiniTip Etch Gel EBS Multi Primer EBS Multi Bond ESPE, Seefeld,
Germany
32% phosphoric acid HEMA, MMC, water Bis-GMA, HEMA, TEGDMA, MAM
Ultraseal XT Plus
Revolution

Fig. 1. (a) Set up of the study divided in SEM/TEM investigation and m-TBS measurement. (b) Set up for m-TBS measurement on ¯attened enamel.
230 R. Frankenberger et al. / Dental Materials 18 (2002) 227±238

thickness of the blade (300 mm) resulting in sticks with a Inc.) to a particle size of 1 mm. Finally the blocks were
cross-sectional area of 700 £ 700 mm (0.5 mm 2). From the treated with 6N hydrochloride acid for 30 s followed by a
resulting 25 central sticks of each tooth, ten were selected 10 min immersion in 2.5% sodium hypochlorite to enable
revealing a distance to the pulp of 2.0 ^ 0.5 mm resulting in the visualization of a three-dimensional interface relief.
20 microtensile specimens for each group (n ˆ 20; Fig. 1a). One further specimen for each enamel group was made
For evaluating enamel bond strength, 18 third molars by etching ¯attened buccal aspects of third molars, applying
were cut longitudinally and the buccal and lingual aspects the same protocol as in the m-TBS study and dissolving the
of the teeth were ¯attened on an area of 4 £ 4 mm without thinned enamel by use of HCl for 3 days resulting in resin
dentin exposure using 600 grit sandpaper under continuous replicas of the etch pattern. The ®nished SEM specimens
water cooling. Then the same specimen preparation proce- were mounted on aluminum stubs (Ted Pella) using adhe-
dure was carried out like in the dentin specimens without sive carbon sticks and a quick drying silver paint (Ted
rubbing of adhesive components. From the resulting 64 Pella).
sticks of each tooth, ten beams with an enamel thickness The specimens were sputter-coated (E 5100, Polaron
of 0.5 ^ 0.1 mm were selected resulting in 20 microtensile Instruments Inc., VG Microtech, Watford, England),
beams in each group (n ˆ 20; Fig. 1b). For the simulation of mounted on aluminum specimen holders to be observed
mixed cavities, also during enamel bonding procedures the under a SEM (4000 £ magni®cation at 15 kV, JSM
primers were applied according to the manufacturer's 6300 V scanning electron microscope, JEOL, Peabody,
recommendations for use. MA, USA). Furthermore the thickness of the adhesive/¯ow-
The sticks were mounted in a Bencor Multi-T device able composite layer above the hybrid layer was measured
(Danville Engineering, Danville, CA, USA) with a special on ten points in the dentin specimens (TiffMes 1.9, Univer-
cyanoacrylate glue (Zapit, Dental Ventures of America, sity of Erlangen).
Corona, CA, USA) and debonded using an universal testing
machine model 4411 (Instron Co., Canton, MA, USA) with 2.4. TEM analysis
a 50-N load cell traveling at a crosshead speed of 1 mm/min.
m-TBS was determined by computing the quotient of maxi- For TEM evaluation of the resin±dentin interfaces, the
mum load (N) and adhesion area. After the m-TBS test, the resin composite layers of the corresponding disk halves
dentin sides of the fractured interfaces were analyzed under were thinned and six small disks with a cross-section area
a stereo light microscope at £ 40 magni®cation to deter- of 1.0±1.5 mm 2 were cut from the central area using a slow-
mine the fracture mode. speed diamond saw under continuous water cooling, to
expose the opposite sides of the interfaces viewed by SEM.
2.2. Statistical analysis Three of the resulting six sticks in each group were then
demineralized in 10% buffered EDTA (pH 7.4) for 72 h and
The statistical analysis was performed using SPSS 8.0 for
consecutively ®xed using 2.5% glutaraldehyde and 2%
Windows (SPSS Inc., Chicago, IL, USA). The mean bond
paraformaldehyde in 0.1 M sodium cacodylate buffer at
strength and margin analysis were non-normally distributed
pH 7.4 for 12 h at 48C. After the ®xation process, the speci-
(as shown by the Kolmogorov-Smirnov test). Therefore,
mens were rinsed with 0.1 M sodium cacodylate buffer at
non-parametric tests were used to compute differences
pH 7.4 for 2 h at 48C. Post-®xation was performed with 2%
between dependent groups (Wilcoxon matched-pairs signed-
osmium tetroxide for 1 h followed by washing in 0.1 M
ranks test) and among independent groups (Mann-Whitney
sodium cacodylate buffer at pH 7.4 for 1 h. After rinsing
U-test, correction method according to Bonferroni-Holm)
in deionized water for 20 min, both the demineralized and
for pairwise comparisons at the 0.05 level of signi®cance
the non-demineralized sticks were dehydrated in ascending
(a ). To assess the in¯uence of the different bonding resins,
grades of ethanol in analogy to the SEM specimens. The
the levels of signi®cance were adjusted to a * ˆ 1-(1 2 a ) 1/k
specimens were then immersed in propylene oxide for
(k ˆ number of performed pairwise tests) [3].
20 min and embedded in a 50/50 mix of propylene oxide
2.3. SEM analysis and epoxy resin (Eponate 12, Ted Pella) in a rotator (Pelco
In®ltrator, Ted Pella) for 6 h at 6 rpm. Finally, the speci-
The disk halves for the resin±dentin interfacial SEM mens were immersed in 100% epoxy resin and set under
investigation (n ˆ 2) were ®xed in 2% paraformaldehyde, vacuum for 12 h for resin in®ltration into the sticks. After
dehydrated in ascending concentrations of ethanol (50±70± positioning of the specimens in rubber molds, the sticks
95±100%) for 1 h, immersed in hexamethyldisilazane were embedded in fresh resin exposing the central aspects
(HMDS, Ted Pella, Redding, CA, USA) and ®nally of the interfaces and dried in an oven for 12 h at 658C. The
embedded in epoxy resin (Epo-Thin, Buehler) exposing blocks were sectioned in an ultra-microtome (MT 2-B Ultra-
the adhesive interfaces of the middle of the tooth. The microtome, Ivan Sorvall Inc., Norwalk, CT, USA) equipped
exposed interfaces were polished with wet silicon carbide with a material science diamond knife (Micro Star Tech-
paper of decreasing abrasiveness (up to 1200 grit) and soft nologies Inc., Huntsville, TX, USA). The demineralized
tissue with increasingly ®ne diamond suspension (Buehler sections were additionally stained with 2% uranyl acetate
R. Frankenberger et al. / Dental Materials 18 (2002) 227±238 231

Table 2
Results of dentin microtensile bond strength [MPa] (SD) for different restorative combinations. Groups with same superscript letters are not statistically
different (Wilcoxon and Mann-Whitney U-test, P . 0.05)

Adhesive system Manufacturer's adhesive Ultraseal XT Plus Revolution

OptiBond FL 33.4 (7.2) A 15.9 (3.4) B 13.3 (4.0) B


Syntac classic 28.8 (8.9) A 11.6 (3.5) B 7.1 (4.1) C
EBS Multi 29.5 (7.7) A 12.5 (5.0) B 8.0 (3.0) C

for 10 min and 3% lead citrate for 5 min. After drying at (Fig. 2c) as well as insuf®cient hybridization of the peritub-
room temperature, the sections were analyzed using a CM- ular and intertubular dentin at the top of the hybrid layer
12 LaB6 Transmission Electron Microscope (Philips Elec- (Figs. 2b, 3b,c, 4b,c). The resin replicas of etched enamel
tronic Instruments, Mahwah, NJ, USA) at an accelerating exhibited a less pronounced formation of resin tags extend-
voltage of 100 kV. ing into acid-conditioned enamel when Revolution was used
for bonding (asterisks in Fig. 5c) compared with Ultraseal
XT Plus and the control specimens (Fig. 5a,b).
The mean layer thicknesses of the adhesives in the control
3. Results
group have been 1.7 ^ 1.6 mm for EBS Multi, 3.2 ^ 1.9 mm
An overview of the results is shown in Tables 2 and 3. for Syntac Classic, and 13.3 ^ 5.7 mm for OptiBond FL.
Both ¯owable resin composites resulted in lower mean The layer thicknesses of the ¯owable composites exhibited
dentin m-TBS when used as bonding resin (11.6± no statistically signi®cant difference and have therefore been
15.9 MPa for Ultraseal XT Plus vs 7.1±13.3 MPa for pooled revealing a mean thickness of 101.8 ^ 44.9 mm for
Revolution; Table 2) compared with the control groups Ultraseal XT Plus and 173.3 ^ 57.1 mm for Revolution. All
(28.8±33.4 MPa; P , 0.05). The different adhesive systems groups have been signi®cantly different from each other
tested exhibited no signi®cant differences in mean m-TBS (layer thickness: EBS , Syntac , OptiBond , Ultraseal ,
(P . 0.05). The failure modes were exclusively adhesive Revolution; P , 0.05).
within the resin±dentin interface. TEM investigation revealed total-etch interfaces for the
For enamel m-TBS, the control groups exhibited no statis- control groups (Fig. 6a) as provided by the literature
tical differences and were between 38.9 and 41.1 MPa and also penetration of the ¯owable composites into acid-
(Table 3). The use of Ultraseal XT Plus as a bonding resin demineralized dentin (Fig. 6b,c). In analogy to the SEM
resulted in similar mean m-TBS (35.4±40.6 MPa) to the observations, ®ller accumulation near the top of the hybrid
control groups (P . 0.05). The application of Revolution layer was clearly evident in the TEM (Fig. 6b,c). Filler
without an intermediate bonding resin resulted in statisti- particles of the diameter of the dentinal tubule entrance
cally lower mean m-TBS to etched enamel (20.8±24.6 MPa; often tended to form plugs and consequently insuf®cient
P , 0.05) than did the original bonding agents and Ultraseal resin tag formation (Fig. 6b,c) like displayed in the SEM
XT Plus. The failure modes detected in the enamel groups ®gures (Figs. 2b, 4b,c).
were adhesive between resin and enamel for the experi-
mental groups. Within the control groups, cohesive failures
in resin were detected (OptiBond FL: 20%, Syntac Classic: 4. Discussion
10%, EBS Multi: 30%) (Table 3).
SEM analysis of the dentin specimens showed a well- The objective of this in vitro study was to clarify whether
de®ned interface of the control groups (Figs. 2a, 3a, 4a), ¯owable resin composites could be used as ®lled adhesives
but also penetration of the ¯owable composites into super- for bonding of resin composites. The method utilized for
®cially acid-demineralized and primed dentin, because a bond strength testing was the microtensile bond test
hybrid layer of similar thickness as in the control groups reported to be well-suited for the evaluation of bond
was clearly evident (Figs. 2b,c, 3b,c, 4b,c). However, closer strengths to enamel and dentin [32±36]. This methodology
investigation exhibited distinct zones of ®ller accumulation provides the possibility to investigate interfacial bond

Table 3
Results of enamel microtensile bond strength [MPa] (SD) and percentages of cohesive failures in enamel for different restorative combinations. Groups with
same superscript letters are not statistically different (Wilcoxon and Mann-Whitney U-test, P . 0.05)

Adhesive system Manufacturer's adhesive Ultraseal XT Plus Revolution

OptiBond FL 40.4 (8.6) A 20% 37.4 (7.1) A 0% 24.6 (5.9) B 0%


Syntac classic 38.9 (9.2) A 10% 35.3 (6.0) A 0% 25.1 (4.5) B 0%
EBS multi 41.1 (10.1) A 30% 40.6 (9.2) A 0% 20.8 (5.8) B 0%
232 R. Frankenberger et al. / Dental Materials 18 (2002) 227±238

Fig. 2. Scanning electron micrographs of resin±dentin interfaces bonded with OptiBond FL. (®nal magni®cation: 4000 £ ). (a) (as per manufacturer's
instructions. The ®lled adhesive (A) penetrates well into the dentinal tubules forming resin tags (T) and various lateral branches (asterisks). The hybrid
layer (H) is approximately 4 mm thick (region between arrowheads). (b) Specimen etched with phosphoric acid, primed with OptiBond Primer and bonded with
Ultraseal XT Plus replacing the OptiBond adhesive (A). Note the porous upper half (hand) of the hybrid layer (H, region between arrowheads). The resin tags
(T) are approximately 10 mm long and show thin endings (asterisks). (c) Specimen etched with phosphoric acid, primed with OptiBond Primer and bonded with
Revolution instead of the OptiBond adhesive (A). The resin tags (T) show lateral branches (asterisk), a hybrid layer (H, between arrowheads) is clearly evident.
Note the accumulation of ®llers and polishing particles at the top of the hybrid layer (right hand) and the gap (left hand) resulting from insuf®cient peritubular
penetration at the tubule entrance.

strengths on small areas below 1 mm 2. Conventional shear tions using the same methodology used in the present study,
and tensile bonding procedures reveal much larger bonding bonding to ¯attened dentin surfaces at variable distances
areas with diameters between 3 and 5 mm [12,33]. When from the pulp, results in regional differences in dentin
dentin is used as a bonding substrate in combination with bond strength [40,41]. Therefore, only the very central
recently developed adhesives reaching bond strengths over areas of the specimens were used to obtain a reliable ran-
15 MPa, these tests often produce non-uniform stresses domization of test specimens. Compared with the results of
resulting in pulling out dentin [37±39]. The observations Shono et al. having involved 50 specimens of different
of the present study indicate that this problem can be occlusal regions per group, the present standard deviations
prevented with microtensile testing because only adhesive are in a comparable range [41]. This consistency demon-
failures were observed for the dentin groups. This con®rms strates the reliability of the modi®ed methodology using 20
the ®ndings of other studies dealing with microtensile test- central specimens in each group providing equal distances
ing [32±35]. As shown by Shono et al. in recent investiga- from the bonded surface to the pulp chamber. According to
R. Frankenberger et al. / Dental Materials 18 (2002) 227±238 233

Fig. 3. Scanning electron micrographs of interfaces bonded with Syntac Classic (®nal magni®cation: 4000 £ ). (a) as per manufacturer's instructions. The
interface shows the adhesive (A), hybrid layer (H, between arrowheads), resin tags (T) and various lateral branches (asterisks). (b) Specimen etched with
phosphoric acid, primed with Syntac Classic Primer/Adhesive and bonded with Ultraseal XT Plus as adhesive instead of the Heliobond adhesive. Note the gap
(asterisks) between hybrid layer (H) and ¯owable resin composite acting as adhesive resin (A). T: resin tags. (c) Specimen etched with phosphoric acid, primed
with Syntac Classic Primer/Adhesive and bonded with Revolution instead of the Heliobond adhesive. Between the top of the hybrid layer (H) and the ¯owable
resin acting as adhesive (A) a distinct gap is detectable (asterisks). Multiple voids (small asterisks) are visible within the applied ¯owable resin composite
forming the tags (T).

the suggestion of Pashley et al., statistics have been carried The bond strength investigation was accompanied with
out with n ˆ 20 as number of specimens under investigation micro-morphological analyses of the resin±dentin interface.
per experimental group [35,35]. SEM analysis of the interfaces displays the resin-side of the
Variation of the bonding substrate is less evident in enamel interface. TEM evaluation of both demineralized and non-
bonding procedures. Nevertheless, the lingual and buccal demineralized specimens represents a complement of the
aspects of the teeth were ¯attened in order to achieve similar investigation at an ultra-morphological level of the
bonding areas. Due to the method involving sticks with a previously tested interfacial characteristics [2,43].
cross-sectional area of 0.5 mm 2, the recorded values for The bonding systems used different priming philosophies
both enamel and dentin bonding are higher compared with according to different solvents. OptiBond FL primer
conventional shear or tensile studies [17,32,33,41]. For the contains water and ethanol, Syntac Classic contains acetone
evaluation of enamel bond strengths, the primers were also and water, and EBS Multi contains water as solvent. Syntac
applied to simulate the situation in cavities, when dentin and classic was used with phosphoric acid etching despite being
enamel are treated simultaneously, but without rubbing, a self-etching primer when used on dentin [44,45]. As repre-
because detrimental effects of scrubbing motions during appli- sentative ¯owable resin composites two materials were
cation on enamel have been reported in the literature [42]. selected because of their different viscosities [46] and
234 R. Frankenberger et al. / Dental Materials 18 (2002) 227±238

Fig. 4. Scanning electron micrographs of interfaces bonded with EBS Multi (®nal magni®cation: 4000 £ ). (a) as per manufacturer's instructions. The hybrid
layer (H) is approximately 4 mm thick (arrowheads), the resin tags (T) exhibit various lateral branches (asterisks). Due to the thin layer of adhesive, the resin
composite (RC) has contact to the hybrid layer (H). (b) Specimen etched with phosphoric acid, primed with EBS Multi Primer and bonded with Ultraseal XT
Plus replacing the EBS Bond. Note the short resin tags (T) and the gap formations at the top of the hybrid layer (H, asterisk) and peritubular at the tubule
entrances (asterisks). (c) Specimen etched with phosphoric acid, primed with EBS Multi Primer and bonded with Revolution as Bonding Agent (A). Note the
partially short resin tags (T, lower asterisk) and the gaps (upper asterisk) at the top of the hybrid layer (H, between arrowheads).

similar radiopacity [47]. Therefore, Ultraseal XT Plus (¯ow: thicker adhesive layers in the OptiBond FL control groups
534 mm 2/30 s at 0.5 MPa [46]) was used as thinner material may have contributed to slightly higher dentin bond
and Revolution (¯ow: 243 mm 2) was used providing a strengths, but this particular difference was not statistically
higher viscosity although it is equally ®lled (both materials signi®cant (P . 0.05; Table 2).
53% by weight [46]) like Ultraseal XT Plus. This way, the Unterbrink and Liebenberg describe the use of Syntac
effect of the consistency was also investigated as there are Single Component with the ¯owable resin composite Tetric
characteristic differences among the numerous ¯owable Flow [31]. However, the adhesive system Syntac Single
resin composites on the market. Component is a one-bottle adhesive combining features of
Another important point when discussing bond strengths primer and bonding resin (which is light-cured), leading to
to dentin is the thickness of the bonding agent hybridization itself. To act as a real ®lled adhesive like
[13,17,21,23,26]. The evaluation of the SEM specimens, OptiBond FL, the dentin should have been acid-etched
however, clearly demonstrated that thicker layers did not and primed with a primer of a two-bottle system (which is
automatically lead to higher microtensile bond strength not light-cured). The ¯owable resin applied after priming
results. In contrast, the ¯owable composites revealed the would play the role of a bonding resin. However, due to its
thickest layers (up to 173 mm due to not possible air- higher viscosity compared with un®lled resins, OptiBond
thinning) and lowest dentin bond strengths. However, the FL adhesive may behave as a ¯owable resin composite.
R. Frankenberger et al. / Dental Materials 18 (2002) 227±238 235

Fig. 5. Resin replicas of composite bonded with EBS Multi (®nal magni®cation 5000 £). (a) as per manufacturer's instructions. The microporosities and
channels provided by acid etching are poured out. (b) Specimen etched with phosphoric acid, primed with EBS Multi Primer and bonded with Ultraseal XT
Plus replacing the EBS Bond. Also all structures of etched enamel are indirectly visible. (c) Specimen etched with phosphoric acid, primed with EBS Multi
Primer and bonded with Revolution as Bonding Agent. Distinct ®ller accumulation prevents the complete penetration of the ¯owable composite into the acid-
conditioned enamel on the left resulting in short resin tags providing less retetion (asterisks).

Therefore, a ¯owable resin composite may have the capabil- strengths. Although there is not much noticeable difference
ity to act in the same way as a ®lled adhesive replacing the between the viscosity of the ®lled adhesive OptiBond FL and
bonding agent of two-bottle systems. The results of the the ¯owable composites during application, there seems to
present study clearly demonstrate that the ¯owable compo- exist a borderline of viscosity avoiding penetration into
sites tested are not capable of hybridizing etched and primed etched and primed dentin. This point of view is supported
dentin as ef®ciently as the commercially available bonding by the fact that the ®lled one-bottle adhesive OptiBond Solo
agents recommended by the manufacturers. (Kerr, Orange, CA, USA) is recently marketed in a lower
In contrast, bonding to enamel shows far less complexity- ®lled formula by the manufacturer. A further explanation
only the penetration into the porosities of acid-etched enamel for the differences in bond strength could be the different
is an prerequisite for successful adhesion [9,10]. The micro- chemical composition of the ®lled adhesive vs the ¯owables
tensile bond strength results reveal that Ultraseal XT Plus marketed primarily as restorative materials.
may act as an enamel bonding agent due to its lower viscos- Penetration of liquids into narrow capillaries, such as the
ity. The viscosity represented by the material Revolution microporosities of etched enamel, is in¯uenced by proper-
seems to be too high for complete penetration into etched ties of the liquid, such as viscosity and the surface free
enamel, as demonstrated by the signi®cantly lower bond energy of the capillary wall [48]. Additionally, viscosity
236 R. Frankenberger et al. / Dental Materials 18 (2002) 227±238

Fig. 6. Transmission electron micrographs of interfaces bonded with OptiBond FL. (a) As per manufacturer's instructions (non-decalci®ed specimen, ®nal
magni®cation: 6300 £ ). H: hybrid layer; Note the complete penetration of the hybrid layer (H) and the `shag carpet'-extension of collagen ®bers into the
adhesive layer (black hand). The small ®llers of the ®lled adhesive penetrate to the entrances of lateral branches (white hand). (b) With Ultraseal XT Plus
replacing the EBS Bond (non-decalci®ed specimen, magni®cation 6,300 £). Note the ®ller particle obstructing the tubule entrance (white hand) and resulting in
short tag formation (black hand). This corresponds to the observations made in Fig. 4b. H: Hybrid layer. (c) With Revolution as bonding agent (decalci®ed
specimen, magni®cation 5000 £ ). Note the ®ller particle clogging the dentinal tubule (arrow) and preventing complete resin tag formation (asterisk) and
hybridization (H) of the demineralized peritubular dentin. The arrow shows a slight `shag carpet' appearance of the top of the hybrid layer resulting from
scrubbing the ¯owable resin composite.

of the restorative resin has been described as a parameter SEM and TEM evaluations corroborate the bond strength
that in¯uences the penetration of restorative resins into acid- results on a micro-morphological level. The SEM speci-
etched enamel [49]. mens show an acid resistant hybrid layer formation in the
Depth of resin penetration into enamel decreases only groups with ¯owable resin composites acting as ®lled adhe-
slightly with increasing viscosity [50]. Several studies sive resins. The detection of accumulated ®llers as well as
have reported that, when applied to acid-etched enamel, polishing particles under the SEM alone would not primar-
there are no signi®cant differences between low-viscosity ily be suspicious for inferior bonding to dentin, and incom-
resins and high-viscosity resins in terms of adaptation and plete resin penetration may not be visible due to the acid
depth of penetration [50±52]. These studies were performed treatment during the specimen production using hydro-
by comparing early-generation high-viscosity composite chloric acid and sodium hypochlorite. The distinct gap
resins with low-viscosity un®lled resins. In fact, composite formations at the top of the hybrid layer, however, indicate
resins seem to adapt themselves to etched enamel surfaces the inferior dentin bonding perfomance of the experimental
equally well as do low-viscosity resins [51]. groups (Figs. 2b, 3b,c, 4b,c). The additional TEM analysis
R. Frankenberger et al. / Dental Materials 18 (2002) 227±238 237

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