Deep Margin Elevation: A Paradigm Shift
Deep Margin Elevation: A Paradigm Shift
Purpose: The purpose of this in vitro study was to compare the shear bond strength of different universal adhesives
to enamel and dentin with and without additional phosphoric acid etching before and after thermocycling (TC).
Materials and Methods: The mesial, distal, lingual, and buccal surfaces of the teeth were ground flat to expose
two enamel areas and two dentin areas. Specimens were randomly divided into 36 groups (n = 10). Four adhesives
were tested: Scotchbond Universal (SBU), Prime & Bond Elect (PBE), All-Bond Universal (ABU), and iBond Universal
(IBU). The application was performed in the self-etch mode (SE) or in the etch-and-rinse mode (ER). Optibond FL
(OFL) was used as an etch-and-rinse control. After composite buildups were made, half of the groups were tested
before and the other half after TC. The failure mode was evaluated using a light microscope.
Results: In enamel, mean bond strengths ranged from 13.4 to 21.9 MPa in the SE mode before TC. When used as
an ER adhesive, mean bond strengths exceeded 30 MPa. TC did not influence the mean bond strengths in either
application mode. Regarding dentin, significant differences in the SE mode were adhesive dependent. Differences
were only detected between SBU and IBU before TC and were not present after TC. When SBU, PBE, and ABU were
used as ER adhesives, no differences were detected before TC. TC only affected IBU when compared to the other
adhesives.
Conclusion: Universal adhesives benefit from phosphoric acid etching, as bond strengths increased especially at
enamel surfaces.
Keywords: universal adhesives, shear bond strength, self-etch, etch-and-rinse, enamel, dentin.
J Adhes Dent 2019; 21: 87–95. Submitted for publication: 30.04.18; accepted for publication: 16.12.18
doi: 10.3290/j.jad.a41974
salts and DCPD.32 In contrast, the functional monomer Four different universal adhesives were tested: Scotch-
glycerol-phosphate dimethacrylate (GPDM) does not form a bond Universal (SBU), Prime & Bond Elect (PBE), All-Bond
stable calcium salt.33 On the other hand, removal of hy- Universal (ABU), and iBond Universal (IBU). Optibond FL
droxyapatite through phosphoric acid etching impairs the (OFL) was used as an etch-and-rinse control adhesive. The
chemical interaction of functional monomers with dentin application of the universal adhesives onto the surfaces
and therefore limits bonding to a solely micromechanical (enamel or dentin) was performed according to the manu-
interaction. As chemical bonding seems to play an impor- facturers’ instructions in the self-etch mode (SE) or with
tant role in the long-term bonding performance of adhesives prior phosphoric acid etching (35%, iBond Etch 35 Gel,
to dentin, hydroxyapatite should be maintained in the hybrid Kulzer; Hanau, Germany) in the etch-and-rinse mode (ER).
layer.28 Universal adhesives may also be used in selective Both enamel and dentin were etched for 15 s before the
enamel-etch or self-etch mode. During this procedure, the application of the adhesives. The composition of the adhe-
smear layer is not removed completely and a hybrid layer sives and their application is shown in Table 1.
consisting of smear layer remnants, apatite crystals, adhe- For the application of the composite, individualized brass
sive monomers, collagen fibrils and minerals is created.2 A rings (inner diameter 3 mm, outer diameter 4 mm, height
major shortcoming when using universal adhesives in self- 2 mm) were used. Composite increments (Venus Diamond,
etch mode is their bond to enamel, which is created by Kulzer) of 1 mm were built up to a total of 2 mm to guaran-
acidic functional monomers. Not only does this lead to tee optimal curing conditions. Each increment was polymer-
lower adhesion to enamel, it also promotes marginal dis- ized for 40 s with an LED curing light (Bluephase, Ivoclar
crepancies and discoloration.13,26 Therefore, it is recom- Vivadent; Schaan, Liechtenstein) at 1100 mW/cm2. Before
mended to selectively etch enamel margins with phosphoric each light-curing cycle, the power output of the LED unit
acid when using universal adhesives.18 was checked with a light meter (Bluephase Meter, Ivoclar
The purpose of this in vitro study was to compare the Vivadent). Half of the groups were stored for 24 h in saline
shear bond strength of different universal adhesives to solution at 37°C before the shear bond strength test was
enamel and dentin with and without additional phosphoric performed. The other half was tested after thermocycling
acid etching before and after thermocycling. The null hypoth- (10,000 cycles of 5°/55°C, dwell time 30 s, transfer time
eses were: 1. Phosphoric acid etching does not increase 10 s). The brass rings were left in place to reduce the
the shear bond strength of universal adhesives to enamel stress at the adhesive interface and the specimens were
or dentin; 2. The shear bond strength of universal adhe- mounted to a computer-controlled universal testing machine
sives to enamel and dentin is not affected by thermocycling. (Type 20K, UTS; Ulm, Germany). The distance between the
crosshead and the tooth surface was 0.1 mm. All speci-
mens were loaded at a crosshead speed of 1 mm/min until
MATERIALS AND METHODS fracture occured. Afterwards, the fractured surfaces were
examined using a light microscope (Stemi SV 6, Zeiss;
Specimen Preparation Jena, Germany) determine the failure pattern: adhesive frac-
For this in vitro study, 180 caries- and restoration-free per- ture at the adhesive interface, cohesive fracture in enamel,
manent human molars were collected and the debris re- dentin, or composite, or mixed fractures (a combination of
moved. The teeth were stored in chloramine-T solution (1%) adhesive and cohesive fractures).
at room temperature until preparation. The use of extracted
human teeth for bond strength testing was approved by the Statistical Analysis
ethics committee of the Hannover Medical School (no. For the statistical analysis, the mean values and the stan-
2092 – 2013). The teeth were embedded in acrylate (Verso- dard deviations were calculated. The level of significance
Cit-2, Struers; Willich, Germany) up to the cementoenamel was set at p < 0.05. The one-way ANOVA was used to com-
junction, so that a right angle was created between the pare the means between the different groups. The t-test
specimen base and the tooth axis. Afterwards, the mesial, was employed to determine statistically significant differ-
distal, lingual, and buccal tooth surfaces were ground flat ences between the means of two unrelated groups. The
to expose two enamel areas and two dentin areas, each significance level was corrected using Bonferroni’s correc-
with a diameter of 4.5 mm at least. For the bonding proce- tion with every additional post-hoc test. In all tests, the ana-
dure, only one dentin area and one enamel area per tooth lyzed groups were homogeneous. Only one variable was dif-
were used for the shear bond strength test. The preparation ferent. The results from the fracture analysis were analyzed
was done using diamond-coated burs (8837.314.014, statistically using cross tabs and the chi-squared test
Brasseler Komet; Lemgo, Germany) and a water-cooled (SPSS 23.0, IBM; Armonk, NY, USA).
high-speed handpiece (300,000 min-1) attached to an align-
ing device to ensure that the preparation was performed
parallel to the tooth axis. Finishing was done with RESULTS
10–40 μm (corresponds to ca 600 grit) Sof-Lex Discs (Sof-
Lex XT 2382M polishing disks, 3M Oral Care; St Paul, MN, One-way ANOVA indicated significant differences between
USA) to create smear layers. The specimens were randomly the adhesives at either enamel or dentin surfaces before
divided into 36 groups (n = 10). and after TC (Table 2).
Prime & Bond Elect 140111 Ultra-mild, 2.5 Mono-, di-, trimethacrylate resins, PENTA, Dentsply; Application PBE and rubbing in for 20 s, Etching of enamel/ dentin for 15 s (35%
(PBE) diketone, stabilizers, organic phosphine Milford, DE, immediately air drying for 5 s, light curing phosphoric acid), rinsing with water (15 s)
oxide, cetylamine hydrofloride, acetone, USA for 10 s. and immediately air drying.
water, HEMA Application and curing: see self-etch
approach.
All-Bond Universal 1400002817 Ultra-mild, 10-MDP, bis-GMA, HEMA, ethanol, water, Bisco; Washing of the surface with water spray, Etching of enamel/ dentin for 15 s (35%
(ABU) 3.1-3.2 initiators Schaumburg, removal of excess water with an absorbent phosphoric acid), rinsing with water,
IL, USA pellet. removal of excess water with an absorbent
Application of two separate coats of ABU in pellet.
a scrubbing mode with a microbrush for Application and curing: see self-etch
10-15 s per coat5 without light-curing approach.
in-between.
Air drying for at least 10 s (surface should
have a uniform glossy appearance,
otherwise, an additional coat of ABU had to
be applied), light curing for 10 s.
iBOND Universal VP180214AK1 Intermediate Methacrylate-monomer (4-META, 10- Kulzer; Hanau, Application of IBU and rubbing in for 20 s, Etching of enamel/ dentin for 15 s (35%
(IBU) strong, 1.8 MDP*), acetone, water *not listed in the Germany Air dry carefully with a gentle oil-free air phosphoric acid), rinsing with water (15 s)
materials MDSD, personal flow until the adhesive fi lm no longer and immediately air drying.
communication with the manufacturer moves. Move the air flow from outside to Application and curing: see self-etch
(Kulzer) inside with increasing intensity at the same approach.
time, if no universally glossy surface
appears, application of a second layer of
IBU, light curing for 10 s.
Optibond FL Primer Primer: ethanol, CQ,HEMA, GPDM, PAMM, Kerr; Biberach, No self-etch approach possible Etching of enamel/ dentin for 15 s (35%
(OFL) 5336245 water Germany phosphoric acid), rinsing with water (15 s)
Adhesive Adhesive: bis-GMA, TEG-DMA, UDMA, and immediately air drying.
5373491 GPDM, CQ, HEMA, filler Primer: rubbing for 15 s, air drying for 5 s.
Adhesive: application and air drying, light
curing for 10 s.
PENTA: dipentaerythritol penta-acrylate phosphate; 4-META: 4-methacryloyloxyethy trimellitate anhydride; 10-MDP: 10-methacryloyloxydecyl dihydrogen phosphate; CQ, camphoroquinone; bis-GMA, bisphenyl-glycidyl-methacrylate;
GDMA: glycerol dimethacrylate; GPDM: glycerol phosphate dimethacrylate; HEMA: 2-hydroxyethyl methacrylate; BPDM: biphenyl dimethacrylate; UDMA: urethane dimethacrylate; PAMM: phthalic acid monoethyl methacrylate.
89
Jacker-Guhr et al
Jacker-Guhr et al
Substrate
Etching
mode
Enamel Enamel Enamel Enamel Dentin Dentin Dentin Dentin
Adhesive SE SE + TC ER ER + TC SE SE + TC ERaA ER + TC
OFL: Optibond FL; SBU: Scotchbond Universal; PBE: Prime & Bond Elect; ABU: All-Bond Universal; IBU: iBond Universal; SE: self-etch mode; ER: etch-and-rinse
mode; TC: thermocycling. Values with different superscript lowercase letters in columns are statistically significantly different. Values with different superscript
uppercase letters in rows are statistically significantly different.
For shear bond strength of enamel without TC, both SBU sive, TC had a significant influence on the mean dentin
and ABU used in self-etch mode showed the highest mean bond strengths (30.6 ± 4.9 vs 21.5 ± 6.1 MPa, p < 0.002)
bond strengths (21.9 ± 7.5 and 19.2 ± 3.1). For SBU, the (Fig 2). No differences were detected within any of the other
mean bond strength was statistically significantly higher adhesives concerning TC, in the etch-and-rinse mode as
than that of PBE (16.1 ± 7.2, p < 0.04) and IBU well as in the self-etch mode (Table 2, Figs 1 and 2).
(13.4 ± 3.7, p < 0.002). ABU (19.2 ± 3.1) showed a statis-
tically significantly higher mean bond strength compared to Fracture Analysis
IBU (13.4 ± 3.7, p < 0.03). On the enamel substrate, adhesive fractures were the most
When used in the etch-and-rinse mode before TC, none frequent type of failure. Regarding the self-etch procedure,
of the universal adhesives produced statistically significant PBE, ABU, and IBU showed 100 % adhesive fractures with
differences from the control (see Fig 1). The lowest mean minor changes induced by TC. Only for SBU was a small
bond strength was measured for IBU, which was statisti- amount of mixed fractures detected before TC (20%). No
cally significantly lower when compared to SBU, ABU, and cohesive fractures were detected in any group (Fig 3). Re-
PBE (33.8 ± 4.8 vs 41.6 ± 4.2, p < 0.005 vs 41.6 ± 4.2, garding the etch-and-rinse approach, there were no statisti-
p < 0.003 and vs 39.1 ± 7.0, p < 0.041, respectively). cally significant differences among fracture patterns. Before
After TC, IBU exhibited the statistically significantly lowest TC, OFL showed varying amounts of adhesive and cohesive
mean bond strength compared to all the other groups fractures, but also up to 50% mixed fractures. After TC,
(32.1 ± 7.4, p < 0.002). However, TC had no influence on statistically significantly more mixed fractures were present
the enamel bond strengths for any of the adhesives used in (90%, p < 0.002, Fig 3).
etch-and-rinse and self-etch modes (Table 2, Fig 1). On the dentin substrate, SBU and PBE used in the self-
Regarding the dentin substrate without TC, only SBU and etch mode resulted in 100% adhesive fractures. The num-
IBU used in the self-etch mode showed statistically signifi- ber of adhesive fractures for ABU and IBU was lower (80%/
cant different bond strength (22.5 ± 6.3 vs 17.1 ± 3.5, 60%). After TC, all groups exhibited mixed fractures. Again,
p < 0.04). No differences were detected between the other no sample fractured cohesively. Regarding the etch-and-
groups in self-etch mode. After TC, there were no statisti- rinse mode, most fractures in all groups were adhesive or
cally significant different mean bond strengths between any mixed, with some exceptions showing cohesive fractures
of the groups, which was also the case when used in self- (all 10%, SBU before TC, PBE and ABU after TC) (Fig 4).
etch mode (Table 2, Fig 2). For SBU in etch-and-rinse mode after TC, 50% cohesive
When used as an etch-and-rinse adhesive, no differ- fractures were recorded for enamel surfaces, whereas for den-
ences were detected before TC with all groups displaying tin, 50% of the fractures were adhesive (p < 0.007, Figs 3 and
mean bond strengths above 30 MPa. After TC, the mean 4). For both groups, the remaining 50% were mixed fractures.
dentin bond strength of IBU decreased to a lower level
when compared to the other groups (21.5 ± 6.1, p <
0.001) (Table 2, Fig 2). DISCUSSION
Before and after TC, all adhesives showed higher mean
bond strengths on both enamel and dentin substrates when The first null hypothesis, that phosphoric acid etching does
used in the etch-and-rinse mode compared to the self-etch not increase the shear bond strength of universal adhe-
mode (p < 0.02). For IBU used as an etch-and-rinse adhe- sives to enamel or dentin, must be rejected. The mean
40.0
30.0
20.0
10.0
40.0
30.0
20.0
10.0
bond strength of both enamel and dentin increased statisti- hesives.10,19 These results are in accordance with our re-
cally significantly by etching with phosphoric acid compared sults, both before and after TC. Therefore, additional
to the self-etch mode. etching of enamel surfaces with phosphoric acid is recom-
Regarding additional phosphoric etching on enamel, in mended for clinical application, as also stated in the IAAD
vitro studies confirmed the improvement of shear and mi- (International Academy for Adhesive Dentistry) working in-
croshear bond strength for both universal and self-etch ad- structions for universal adhesives.18
Fig 3 Bar graph depicting the percentages of adhesive, cohesive and mixed fractures in enamel.
Fig 4 Bar graph depicting the percentages of adhesive, cohesive, and mixed fractures in dentin.
As previously demonstrated by other authors27,31 for chesi et al12 did not find any differences between the bond
self-etch adhesives with additional phosphoric-acid-etching, strengths obtained in the self-etch or etch-and-rinse mode
additional use of phosphoric acid on dentin prior to the ap- in dentin. These results disagree with the present findings,
plication of universal adhesives results in deeper penetra- where all tested universal adhesives showed significantly
tion and formation of thicker hybrid layers. Nevertheless, in higher mean shear bond strengths after additional phos-
contrast to the present results, mean bond strength did not phoric acid etching of dentin surfaces before thermocycling
increase significantly. Furthermore, Chen et al2 and Mar- (Table 2, Fig 2). Zhang et al37 showed significantly higher
microtensile bond strengths for All-Bond Universal when increased water absorption within the hybrid layer, which
used in the etch-and-rinse mode, even after aging for 12 might jeopardize stable and durable adhesion,19 HEMA im-
months. In the current study, after thermocycling, 3 out of proves the wetting ability of the dentin. HEMA-free IBU, when
4 universal adhesives showed a higher shear bond used as an etch-and-rinse adhesive, showed dentin bond
strength, with the exception of IBU (17.5 ± 1.7 self-etch vs strengths before TC which were not significantly different
21.5 ± 1.9 etch-and-rinse; p < 0.128) (Table 2, Fig 2). A from those of the other universal adhesives. However, IBU
recent meta-analysis21 including 10 publications (since Oc- revealed the lowest bond strengths after TC. Moreover, the
tober 2014) on the bond strength of universal adhesives HEMA-containing adhesive SBU showed statistically signifi-
found that better dentin bond strength was achieved by pre- cantly better adhesion than IBU (Fig 2). These findings are in
vious phosphoric acid etching for the ultra-mild universal contrast to previous research, which showed that the func-
adhesive All-Bond Universal (pH = 3.1), which is in agree- tional monomer HEMA significantly reduced nano-layering.35
ment with the present results. The meta-analysis results However, it should be noted that in this in vitro study,
were supported by the bond strength of PBE (pH = 2.5) and enamel and dentin were treated separately; therefore, the
SBU (pH = 2.7) in the current study (Fig 2). The reason for technique sensitivity of the etch-and-rinse procedure, which
this result might be that the ultra-mild adhesive was not may be relevant in a clinical situation, was not considered
able to etch sufficiently through the smear layer covering in the test setup. Small class I and II cavities in particular,
the dentin to dissolve it.21 On the other hand, additional in which the phosphoric acid might quickly spread to the
etching of the dentin with phosphoric acid may lead to ex- dentin in an uncontrolled manner during a selective-enamel-
cessive demineralization. As calcium is removed from den- etch procedure, are a major challenge for the operator.23
tin, a network of collagen fibers surrounded by water is cre- Therefore, moisture management in dentin is not only de-
ated. The loss of calcium might inhibit the ionic bonding pendent on the substrate itself but also on the operator
between calcium and the phosphate and/or carboxylate and his/her expertise.24,31 Apart from pre-etching with
groups in the adhesive.20 If excessive demineralization oc- phosphoric acid, the shear bond strength of universal adhe-
curs, the adhesive is no longer able to infiltrate the entire sives can be improved by using the “double layer tech-
depth of the demineralized dentin. As a consequence, col- nique”.7,25 However, Taschner et al25 showed that the bond
lagen hydrolysis may occur on the bottom of the hybrid strength of one-step self-etch adhesives when using the
layer, which can result in adverse effects. This observation double layer technique depends on the adhesive, which
was also made by Hanabusa et al,8 who detected more should be taken into consideration.
defects in the hybrid layer after additional phosphoric acid Thermocycling and water storage can decrease the mean
etching compared to self-etch application. However, these bond strengths of adhesives. Our second null hypotheses,
findings are not supported by the results of the present which stated that the bond strength of universal adhesives
study, as phosphoric acid etching statistically significantly is not affected by thermocycling, must be rejected. For
improved the dentin bond strength. enamel, TC had no influence on the shear bond strength,
Regarding their chemistry, universal adhesives per se do independent of the etching mode (self-etch vs etch-and-
not require a separate etching step because they contain rinse, Fig 1). Regarding dentin, only one of the tested uni-
different acidic monomers. Most of the universal adhesives versal adhesives (IBU: without TC 30.6 ± 4.9 vs with TC
contain the functional monomer 10-MDP (10-methacryloyl- 21.5 ± 6.1) was affected by TC when used in the etch-and-
oxydecyl dihydrogen phosphate) or other functional mono- rinse mode, resulting in a shear bond strength decrease of
mers such as 4-META, GPDM, PENTA, 4-MET.12,14 These about 30% after TC. One explanation for this might be the
monomers enable universal adhesives to be used in multi- application mode used with IBU in this study. According to
mode applications, meaning with the self-etch, selective- the manufacturer’s instructions, it should be used in one
enamel etch or etch-and-rinse technique.23 Among all func- layer and air dried until the adhesive film no longer moves.
tional monomers, 10-MDP is of particular importance No second layer was applied (which is optional according to
because it establishes a chemical bond to dentin via its the manufacturer’s instructions), because a glossy surface
phosphate group, which binds ionically to residual calcium was already achieved with one layer. Nevertheless, the
attached to the collagen fibers.32,36 Munoz et al15 found manufacturer’s instructions for this step are less precise
that 10-MDP seems to preserve the bond strength after ar- when compared to the other tested adhesives, where air
tificial aging with water compared to non-MDP-containing drying time and number of coats were described in detail.
universal adhesives. The reason for this effect might be the As the present study followed the requirement for a glossy
formation of a stable and water-resistant Ca-monomer salt surface/motionless adhesive film and not a specific air dry-
created by the reaction of 10-MDP and the Ca2+ ions of hy- ing duration for IBU, a rather pronounced oxygen inhibition
droxyapatite.6,34 Our results confirm this, as the shear layer over a thin hybrid layer may have been formed and
bond strength to dentin remained stable after thermocycling weakened the bond strength after aging. Velazquez et al30
for all universal adhesives. All universal adhesives tested in compared adhesives which were modified by adding benzoyl
this study contained different functional monomers: peroxide and thus transformed from light-curing to dual-
4-META, 10-MDP and PENTA (Table 1). curing adhesives. They stated that the lower bond strength
Some universal adhesives also contain the hydrophilic after solely light curing compared to dual curing was caused
monomer HEMA (2-hydroxyethyl methacrylate). Apart from by oxygen inhibition, which may have been even more pro-
26. Tay FR, Pashley DH. Have dentin adhesives become too hydrophilic? J 35. Yoshida Y, Yoshihara K, Hayakawa S, Nagaoka N, Okihara T, Matsumoto
Can Dent Assoc 2003;69:726-731. T, Minagi S, Osaka A, Van Landuyt K, Van Meerbeek B. HEMA inhibits in-
27. Van Landuyt KL, Kanumilli P, De Munck J, Peumans M, Lambrechts P, terfacial nanolayering of the functional monomer MDP. J Dent Res
Van Meerbeek B. Bond strength of a mild self-etch adhesive with and 2012;91:1060-1065.
without prior acid-etching. J Dent 2006;34:77-85 36. Yoshida Y, Yoshihara K, Nagaoka N, Hayakawa S, Torii Y, Ogawa T,
28. Van Landuyt KL, Yoshida Y, Hirata I, Snauwaert J, De Munck J, Okazaki Osaka A, Van Meerbeek B. Self-assembled nano-layering at the adhesive
M, Suzuki P, Lambrechts B, Van Meerbeek B. Influence of the chemical interface. J Dent Res 2012;91:376-381.
structure of functional monomers on their adhesive performance. J Dent 37. Zhang Z, Tian F, Niu L, Ochala K, Chen C, Fu B, Wang X, Pashley DH, Tay
Res 2008;87:757-761. FR. Defying ageing: An expectation for dentine bonding with universal ad-
29. Van Meerbeek B, Perdigão J, Lambrechts P, Vanherle G. The clinical per- hesives?. J Dent 2016;45:43-52.
formance of adhesives. J Dent 1998;26:1-20.
30. Velazquez E, Vaidyanathan J, Vaidyanathan TK, Houpt M, Shey Z, Von
Hagen S. Effect of primer solvent and curing mode on dentin shear bond
strength and interface morphology. Quintessence Int 2003;34:548-555.
31. Wagner A, Wendler M, Petschelt A, Belli R, Lohbauer U. Bonding perfor-
mance of universal adhesives in different etching modes. J Dent
2014;42:800-807.
32. Yoshihara K, Hayakawa S, Nagaoka N, Okihara T, Yoshida Y, Van Meer-
beek B. Etching efficacy of self-etching functional monomers. J Dent Res
2018;97:1010-1016. Clinical relevance: Pre-etching of enamel with phos-
33. Yoshihara K, Nagaoka N, Hayakawa S, Okihara T, Yoshida Y, Van Meer-
beek B. Chemical interaction of glycerol-phosphate dimethacrylate phoric acid increased the shear bond strength of univer-
(GPDM) with hydroxyapatite and dentin. Dent Mater 2018;1072-1081. sal adhesives before and after thermocycling. As a con-
34. Yoshida Y, Nagakane K, Fukuda R, Nakayama Y, Okazaki M, Shintani H, sequence, this procedure can be recommended clinically
Inoue S, Tagawa Y, Suzuki K, De Munck J, Van Meerbeek B. Comparative
study on adhesive performance of functional monomers. J Dent Res when using this new class of adhesives.
2004;83:454-458.