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d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

available at www.sciencedirect.com

journal homepage: www.intl.elsevierhealth.com/journals/dema

Review

Relationship between bond-strength tests and clinical


outcomes

B. Van Meerbeek ∗ , M. Peumans, A. Poitevin, A. Mine, A. Van Ende, A. Neves,


J. De Munck
Leuven BIOMAT Research Cluster, Department of Conservative Dentistry, School of Dentistry, Oral Pathology and Maxillo-Facial Surgery,
Catholic University of Leuven, Kapucijnenvoer 7, B-3000 Leuven, Belgium

a r t i c l e i n f o a b s t r a c t

Article history: One often alleges that laboratory bond-strength testing cannot predict clinical effectiveness
Received 19 November 2009 of adhesives. Major argument to sustain this claim is the wide variation in bond-strength
Accepted 19 November 2009 values recorded for one specific adhesive among different research institutes worldwide.
The main reason for these inconsistent bond-strength measurements is supposedly the
current lack of a standard bond-strength testing protocol. This paper (and presentation)
Keywords: aimed to report on an extensive literature review with regard to the different laboratory
Review bond-strength test methods and their data provided, along with a second extensive litera-
Bond strength ture review on clinical effectiveness data of adhesives in terms of retention rates of adhesive
Clinical effectiveness Class-V restorations. Combining both systematic reviews, we have subsequently searched
Clinical trial for a potential relationship between bond-strength data and clinical outcomes.
Retention © 2009 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.
Adhesive

Contents

1. Dental adhesive technology ANNO 2009. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e101


1.1. Etch&rinse. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e101
1.2. Self-etch . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e101
1.3. Self-adhesive . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e103
2. Measuring bond strength . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e104
2.1. Macro-shear . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e105
2.2. Macro-tensile/push-out . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e105
2.3. Micro-tensile . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e105
2.4. Micro-shear . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e107
2.5. Fatigue . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e107
2.6. Bond durability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e107
2.7. KULeuven systematic review on bond strength . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e108
2.8. Fracture mechanics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e109


Corresponding author. Tel.: +32 16 33 75 87; fax: +32 16 33 27 52.
E-mail address: bart.vanmeerbeek@med.kuleuven.be (B. Van Meerbeek).
0109-5641/$ – see front matter © 2009 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.dental.2009.11.148
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e101

3. Assessment of sealing ability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e109


3.1. Micro-leakage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e109
3.2. Marginal adaptation/gap formation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e109
3.3. Bacterial leakage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
3.4. Permeability . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
3.5. Nano-leakage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
3.6. 3D-leakage . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
4. Clinical performance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
4.1. Class-V clinical data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e110
4.2. KULeuven systematic review on Class-V clinical data, Part I . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e113
4.3. KULeuven systematic review on Class-V clinical data, Part II . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e114
5. Relationship between laboratory and clinical bonding effectiveness . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e114
5.1. Relationship I . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e115
5.2. Relationship II. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e115
5.3. Relationship III . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e115
5.4. Relationship IV . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e115
6. Conclusions and closing remarks . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e116
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e116
References. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . e116

step following a 3-step procedure. The final objective is to


1. Dental adhesive technology ANNO 2009 micro-mechanically interlock upon diffusion and in situ poly-
merization of monomers into the enamel etch-pits (Fig. 1a),
The fast progress in dental adhesive technology has exten-
the opened dentin tubules and the exposed collagen network,
sively influenced modern restorative dentistry. Although
the latter forming the well-documented hybrid layer (Fig. 2a).
decayed/fractured teeth can be reconstructed minimal-
Without doubt, the micro-mechanical interlocking of tiny
invasively and nearly invisibly using adhesive technology, the
resin tags within the acid-etched enamel surface is still today
clinical longevity of composite restorations is today still too
the best achievable bond to enamel [6–8]. It not only effec-
short [1,2]. Despite the enormous advances made in adhesive
tively seals the restoration margins on the long term, but also
technology during the last 50 years, the bonded interface itself
protects the more vulnerable bond to dentin against degrada-
remains the Achilles heel of an adhesive filling [3,4]. Mainly
tion [9]. On the contrary, etching dentin is a rather aggressive
water sorption is thought to destabilize the adhesive–tooth
procedure as it dissolves and removes (through rinsing) the
bond, though the actual interfacial degradation mechanisms
natural protection of collagen (Fig. 2a), thereby producing a
are far from understood. In this context, several aspects
resin–collagen complex that is vulnerable to degradation upon
should be considered with regard to the strength and dura-
water sorption, possibly enhanced by the documented enzy-
bility of the bond to the two dental hard tissues, enamel and
matic degradation process [10–12]. As the most intimate and
dentin. These include the heterogeneity of tooth structure and
stable intermolecular interaction possible, primary chemical
composition, the features of the dental surface exposed after
interaction between resin and the mainly organic substance
cavity preparation, and the characteristics of the adhesive
remaining at acid-etched dentin would definitely contribute to
itself, such as its strategy of interaction with both substrates
the bond durability, but is however lacking [13,14]. This defi-
and its basic physicochemical properties. Furthermore, all
cient chemical interaction should most likely be regarded as
sorts of chemical and mechanical challenges that are inher-
the major shortcoming of today’s etch&rinse approach. Never-
ent to the oral environment should be taken into account,
theless, traditional 3-step etch&rinse adhesives are still today
such as there are moisture, masticatory stresses, changes in
regarded as ‘gold-standard’.
temperature and pH, and dietary and chewing related habits
[5].
Modern adhesive approaches can be divided into (1) an 1.2. Self-etch
etch&rinse, (2) a self-etch (or etch&dry), and (3) nowadays also
a self-adhesive approach [6]. The self-etch approach can be further subdivided into a
‘strong’ (pH < 1), an ‘intermediately strong’ (pH ≈ 1.5), a ‘mild’
1.1. Etch&rinse (pH ≈ 2), and an ‘ultra-mild’ (pH ≥ 2.5) self-etch approach
depending on the self-etching or demineralization intensity
In brief, the multi-step etch&rinse approach involves a phos- [15]. Self-etching only dissolves the smear layer, but does not
phoric acid-etch step that at enamel produces deep etch-pits remove the dissolved calcium phosphates, as there is no rinse
in the hydroxyapatite (HAp)-rich substrate, and at dentin dem- phase. The more intense the self-etching, the more calcium
ineralizes up to a depth of a few micrometers to expose a phosphates are dissolved and embedded within the interfacial
HAp-deprived collagen mesh. The next step involves either transition zone [16]. Such resin-encapsulated calcium phos-
a separate priming step followed by the application/curing phates within the exposed collagen mesh are however rather
of a combined primer/adhesive resin following a simplified soluble (Fig. 3) and may explain the lower laboratory and clin-
2-step procedure, or a separate primer and adhesive resin ical bonding performance of strong self-etch adhesives, in
e102 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

Fig. 1 – TEM photomicrographs illustrating the adhesive–enamel interface for an etch&rinse (a) versus a ‘mild’ self-etch
adhesive (b). Note the partially dissolved HAp-crystals and much deeper interaction at phosphoric-acid-etched enamel
(following the etch&rinse approach in (a)) versus the visibly hardly ‘touched’ HAp-structure and superficial but tight
interaction at self-etched enamel (following the mild self-etch approach in (b)). The white porosities in between the
HAp-crystals (b) should be regarded as an artifact due to the diamond knife-sectioning procedure through the brittle enamel
substrate.

Fig. 2 – TEM photomicrographs illustrating the adhesive–dentin interface for an etch&rinse (a) versus a ‘mild’ self-etch
adhesive (b), taken after heavy-metal staining and at the same magnification. While the etch&rinse approach (using 30–40%
phosphoric acid) exposes collagen deeply (a), all collagen remained protected by HAp following the mild self-etch approach (b).
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e103

MDP appeared not only more effective, but also more stable in
water than that provided by other functional monomers like
4-MET (4-methacryloyloxyethyl trimellitic acid) and phenyl-
P (2-methacryloyloxyethyl phenyl phosphoric acid), in this
order [22]. The dissolution rate of the respective calcium salts
of these three monomers, as measured by AAS (or atomic
absorption spectroscopy), was inversely related to their chem-
ical bonding potential revealed by XPS: the more intense the
chemical bonding potential, the less the resultant calcium salt
could be dissolved. This finding was further explained in the
‘AD-concept’ or the adhesion–decalcification concept that dic-
tates if molecules will either adhere to or decalcify mineralized
tissues [28,29].
Two-step self-etch adhesives involve the application of
a separate, more hydrophobic adhesive resin after the
Fig. 3 – TEM photomicrograph illustrating the hydrophilic self-etch primer. This makes the interface more
adhesive–dentin interface produced by a ‘strong’ self-etch hydrophobic and thus better seals it to the direct benefit of
adhesive. Besides deep hybridization, typical of such an bond durability. Finally, the most simple- and fast-to-use 1-
adhesive are the intensely stained interfibrillar spaces in step (self-etch) adhesives generally come with some sacrifice
between the exposed collagen fibrils of the hybrid layer, in bonding performance. This lower bonding efficiency has
most likely representing dissolved calcium phosphates. been thoroughly documented in laboratory research, and must
be ascribed to, among others, to a lower polymerization con-
version and thus inferior mechanical properties, enhanced
water sorption through osmosis from the host dentin, poten-
particular to dentin [17]. At enamel, they however perform in tial phase-separation effects when the adhesive solution is
general much better due to this more aggressive self-etching low in or free of HEMA (2-hydroxyethyl methacrylate), filler de-
[18]. The less intense the self-etching, the more bur-smear bonding within the adhesive resin through hydrolysis of the
may interfere with the eventual bonding performance (Fig. 4) silane coupling, potential smear interference for ultra-mild
[19,20]. In particular ‘mild’ (pH ≈ 2) self-etch adhesives appear self-etch adhesives, and reduced shelf life in particular with
to deal reasonably well with bur-smear, producing a submi- regard to one-component formulations [30–35].
cron hybrid layer with substantial HAp-crystals still protecting
the collagen fibrils (Fig. 2b). Functional monomers, in par- 1.3. Self-adhesive
ticular like 10-MDP (10-methacryloyloxydecyl dihydrogen
phosphate), have been proven to interact with this resid- Glass-ionomers and resin-modified glass-ionomers are ‘self-
ual HAp through primary ionic binding [21,22]. The resultant adhesive’ through submicron hybridization, combined with
twofold micro-mechanical and chemical bonding mechanism well-proven primary ionic interaction of polyalkenoic acid
closely resembles that of glass-ionomers (Fig. 5; see below) with calcium within HAp (Fig. 5). Polyalkenoic acid possesses
[6,21,23–27]. However, chemical bonding potential on its own abundant functional carboxylic groups that ‘grab’ HAp simul-
is insufficient; the formed ionic bonds should also be stable in taneously at different and remote sites. Other ‘self-adhesive’
an aqueous environment. Chemical bonding promoted by 10- materials are the so-called self-adhesive luting composites

Fig. 4 – TEM photomicrographs showing the resin–smear complex at the interface of an ‘ultra-mild’ self-etch adhesive
bonded to enamel in (a) and to dentin in (b).
e104 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

electron microscopy (potentially supplemented with chemical


interfacial analysis) definitely reveals a deeper insight in the
underlying mechanisms of adhesion, the actual bonding effec-
tiveness of today’s adhesive approaches should be measured
using a mechanical bond-strength test.

2. Measuring bond strength

By definition, the ideal bond-strength test should be in the


first place easy (meaning low technique-sensitivity) and rel-
atively fast. In general, advantages of ‘laboratory testing’ are,
among others, (1) the quickness to gather data on a specific
parameter/property, (2) the relative ease of the test method-
Fig. 5 – TEM photomicrograph illustrating the twofold ology commonly used, (3) the possibility (and necessity) to
‘self-adhesive’ mechanism of (resin-modified) measure one specific parameter, while keeping all other
glass-ionomers, consisting of micro-mechanical variables constant, (4) to be able to directly compare the per-
interlocking through submicron hybridization, along with formance of a new and/or experimental material/technique
primary electrostatic binding of the carboxyl groups of with that of the current ‘gold-standard’, (5) to be able to test
polyalkenoic acid as the principal functional polymer with simultaneously many (of course within certain limits) exper-
the glass-ionomer formulation to HAp. imental groups within one study set-up, and (6) to be able
to mostly use relatively unsophisticated and inexpensive test
protocols/instruments. The final objective of a laboratory test
that have been introduced some years ago [36–38]. They are should obviously be to gather data in prediction of the eventual
often mistakenly termed as ‘self-etching’, while they inter- clinical outcome.
act only very superficially with dentin without clear signs of In order to measure the bonding effectiveness of adhesives
demineralization (Fig. 6). Finally, it is in the line of expecta- to enamel and dentin, diverse methodologies can today be
tions that such self-adhesive luting composites will soon lead used [39]. The bond strength can be measured statically using
to the development of self-adhesive flowable and later full- a MACRO- or MICRO-test set-up, basically depending upon the
restorative composites. size of the bond area. The MACRO-bond strength, with a bond
While adhesive–enamel/dentin interfacial characteriza- area larger than 3 mm2 , can be measured in ‘shear’, ‘tensile’,
tion using scanning and even more reliably using transmission or using a ‘push-out’ protocol.

Fig. 6 – TEM photomicrographs illustrating the interface of a self-adhesive luting composite to either fractured (and thus
smear-free) dentin in (a) and to bur-cut dentin in (b).
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e105

2.1. Macro-shear over, 3-step etch&rinse adhesives outperformed the 2-step


etch&rinse adhesives, and they on their turn the 2-step self-
Definitely most commonly used is the shear bond-strength etch adhesives that presented with a pooled bond strength
technique [39]; it was found to have been used in 26% of that was not statistically significant from that recorded for
scientific papers reporting on bond strength. As no further the most simple-to-use 1-step adhesives. The significantly
specimen processing is required after the bonding procedure, highest bond strength was measured for OptiBond FL (Kerr,
the shear bond-strength test undoubtedly thanks its high pop- Orange, CA, USA) that somewhat surprisingly performed only
ularity in companies and other research institutes as it is the not significantly better than the relatively new 1-step adhesive
most easy and fastest method. In an attempt to standard- Easy Bond (3M ESPE, Seefeld, Germany). Very striking is also
ize the test protocol, specific jigs have been prepared, such the operator effect, widely varying for each product. Indeed,
the Ultradent jig (Ultradent, Salt Lake City, UT, USA) and the very pertinent information gathered in this mega-test is the
more recent SDI rig (SDI, Bayswater, Victoria, Australia) (Fig. 7). coefficient of variance that gives some idea on the technique-
Despite such standardization attempts, a meta-analysis of sensitivity of individual products. Products that presented
factors involved in bond-strength testing revealed the signifi- with the highest bond strength, were not necessarily the least
cant influence of various parameters, like those related to the technique-sensitive. Care should nevertheless be taken not to
dentin substrate (i.e. nature of teeth), to the composite and over-interpret the data, this in the first place because of the
bonding area (i.e. composite stiffness), to the storage condi- shear bond strength set-up (see above) and in particular also
tions of the bond assemblies (i.e. thermo-cycling), and to the because of the solely ‘immediate’ bond-strength data recorded
test design (i.e. crosshead speed) [40]. In particular, a strong without any kind of bond aging involved (see below).
correlation was found between the mean bond strength and
the failure mode: the higher the bond strength, the higher the 2.2. Macro-tensile/push-out
rate of cohesive failure. Also the type of composite is crucial.
A stiffer composite will result in different stress distributions Less popular is a macro-tensile bond-strength approach that
at the interface and lead to a higher apparent bond-strength nevertheless can be used to measure for instance the bond
value. Our extensive literature review conducted on the occa- strength of cements to hard materials such as ceramics and
sion of this presentation at the Portland Academy of Dental metal alloys [51,52]. A push-out approach has also been
Materials (ADM) meeting (see below) revealed a positive cor- employed, in particular to dynamically test the fatigue resis-
relation between bond strength and the E-modulus of the tance of adhesive–dentin bonds [53–56]. It has however never
composite used [41,42]. Somewhat surprisingly, adhesives are been adopted as a universal bond-strength test method, most
quite often tested in bond-strength studies along with the likely because of the more laborious specimen preparation
respective composite of the same company in the sense that involved as well as the more time-consuming methodology.
the composite was fine-tuned to the adhesive (or vice versa). This method appeared however very useful to test the reten-
While this may be true to a certain extent, doing so, conclu- tion of posts luted in root canals [55,56].
sions can only be drawn at the level of the adhesive/composite
combination, and certainly not at the level of the adhesive 2.3. Micro-tensile
itself. Another source of variability are the different configura-
tions employed to apply the shear force, including wire loops, Common MICRO-bond strength is typically measured in
points and knife edges [43]. In particular, the use of a wire loop tensile, as micro-tensile bond-strength testing (␮TBS) was
for shear bond-strength tests appeared to concentrate stress developed in 1994 by Sano et al. [57]. The bond area tested
more near the interface rather than a knife edge. is much smaller compared to that of the ‘MACRO’ tests, being
The most frequently ignored guideline in the test pro- about 1 mm2 or less. After the bonding procedure, some fur-
tocol following the ISO/TS 11405 specification (2003) is that ther specimen processing or the actual preparation of the
‘a limitation of the bonding area is important’ [44]. Many micro-specimens is required, rendering the test more labo-
times, the adhesive is applied to the entirely exposed rious and technique-sensitive. Nevertheless, a long list of
enamel/dentin substrate, by which the bonding area is not advantages is typically ascribed to ␮TBS when compared to
only substantially larger, but also the shear load is applied macro-bond-strength testing, of which the most important
to the adhesive–composite interface rather than to the are the better economic use of teeth (with multiple micro-
adhesive–tooth interface (Fig. 7). Besides such major flaws in specimens originating from one tooth), the better control of
the test protocol, there is a good consensus in current litera- regional differences (e.g. peripheral versus central dentin),
ture that the shear stress is not uniformly distributed across the better stress distribution at the true interface (avoid-
and not necessarily focused at the true interface [43,45–48]. ing cohesive failure in tooth substrate or composite), etc.
Nevertheless, the shear bond-strength test probably [57,58]. This renders the ␮TBS test more versatile, as multiple
remains a very popular test to screen new adhesive formu- specimens obtained from a single tooth enable more inven-
lations on their bonding effectiveness. The most noteworthy tive study set-ups and better controlled substrate variables.
example of shear bond-strength testing is the ‘Battle of However, several micro-specimen preparation protocols are
Bonds’ series by Degrange et al. [49,50]. A gigantic dataset being used worldwide, one being more technique-sensitive
of more than 16,000 ‘immediate’ bond strengths to dentin than the other. Today, so-called ‘trimmed’ and ‘non-trimmed’
was collected, and revealed upon pooling of the data per micro-specimens are prepared, both having advantages and
adhesive class a statistically significant higher bond strength disadvantages [59,60]. Non-trimmed micro-specimens are
of etch&rinse adhesives than of self-etch adhesives. More- definitely most easy and fast to prepare. Trimming the micro-
e106 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

Fig. 7 – Figure showing the Ultradent jig (top) and the SDI rig (bottom), both specifically designed and fabricated for shear
bond-strength testing. An inappropriate, though commonly used specimen-preparation technique involves the application
of the adhesive to the entire tooth surface, on top of which a composite cylinder is bonded (top). As shown by the fractured
specimen (top right), the shear stress caused the specimen to de-bond at a much larger area than the area to which the
composite cylinder was bonded. The SDI rig much better enables both the adhesive and the composite be applied to a
confined area (bottom).

specimens at the interface to so-called hourglass-shaped then use linear mixed models (ANOVA with random effects)
specimens better concentrates stress at the interface, but to analyze the data. As also recommended by the ISO Tech-
involves a more invasive specimen procedure. When this nical specification on testing adhesion to tooth structure (ISO
trimming is not carefully performed, interfacial defects may No. 11405, 2003) [44], another way would be to apply survival
easily be introduced and early set off crack-propagation dur- analysis like the Weibull model or Cox proportional hazard
ing the tensile loading of the micro-specimen, eventually using the force that is required for bond failure [66]. Although
causing the interface to fail prematurely at a lower (bond) not generally agreed upon, a minimum of 5 teeth seems rea-
strength [61]. Originally, interfaces were trimmed by free hand sonable in order to keep the advantage of more economic use
using a dental handpiece [57,62]. Despite being very labori- of teeth using a ␮TBS approach.
ous, such micro-specimen trimming largely depends on the A second issue involves the hard-to-neglect amount of
skills of the operator, thereby introducing a learning curve pre-testing failures often recorded with micro-tensile bond-
and non-negligible factor of technique-sensitivity. Therefore, strength testing [65]. Several approaches have been applied to
semi-automatic trimming of micro-specimens using a so- deal with the pre-testing failures: (a) exclude all pre-testing
called MicroSpecimen Former (University of Iowa, Iowa City, failures from further (statistical) analysis, which obviously
IA, USA) is highly advisable to trim rectangular specimens in overestimates the actual bond strength; (b) assign a bond-
a well-controlled and standardized way into specimens with a strength value of for instance 0 MPa to each pre-testing failure.
circular cross-section. Also other factors such as specimen–jig This actually penalizes the product too severely, as there was
attachment, specimen-loading speed and specimen align- a certain bond strength; and (c) a modification of the for-
ment, do influence the final outcome, and therefore should mer approach by assigning a pre-determined value to each
be standardized within the test set-up [58,63,64]. pre-testing failure, as for example the lowest ␮TBS measured
One major issue of dispute in current literature is the within the respective group [66–68]. Apart from the obvious
required number of individual teeth from which many micro- effect on the mean ␮TBS value, these data transformations
specimens can be prepared to be statistically sound [65]. An may also affect the subsequent statistical analysis. Especially
elegant way to handle this problem is to use every tooth as its in case of many pre-testing failures, methods (b) and (c) will
own control. This means that the tooth surface for bonding is result in a data distribution that is inevitably skewed. As a
divided into 2 or, for practical reasons, a maximum of 4 sectors, result, more powerful parametric statistical analyses cannot
each receiving a different treatment. Probably, the best way is be applied anymore and one has to rely on more basic non-
to know which micro-specimen comes from which tooth, and parametrical methods such as the Kruskall–Wallis test. Just
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e107

ignoring pre-testing failures, following method (a), should not need for more fatigue testing of adhesives and even though
be done (perhaps except when the micro-specimen failed several typical fatigue phenomena can be observed (Fig. 8)
remote from the interface in one of the adherents), as a high [72,78], little new information on bonding effectiveness is
proportion of pre-testing failures is typically associated with provided than that revealed by the easier and faster static
low ␮TBSs measured for the other micro-specimens that did bond-strength tests. For example, micro-rotary [79] as well as
not de-bond prior to testing [65]. Moreover, adhesives that con- micro-tensile fatigue testing [84,85] revealed a similar superior
sistently present with relatively high ␮TBSs, do not suffer from bonding effectiveness of the 3-step ‘gold-standard’ etch&rinse
pre-testing failures. Eventually, micro-specimen processing adhesive OptiBond FL (Kerr) over the 2-step ‘gold-standard’
should be as a-traumatic as possible and the use of special self-etch adhesive Clearfil SE Bond (Kuraray, Tokyo, Japan), that
measures to avoid pre-testing failures, such as the use of on its turn bonds significantly better than the 1-step adhesive
alginate or gypsum to fill up the space between the slabs, G-Bond (GC, Tokyo, Japan). In addition, these fatigue tests have
thereby better supporting the slabs during the second 90- largely been applied to dentin with bonding to enamel being
degree-turned cut, is highly advisable. much more difficult to assess in fatigue.
Although hard to scientifically prove, a micro-tensile proto-
col appears to be able to discriminate adhesives better on their 2.6. Bond durability
bonding performance than a traditional shear bond-strength
approach (see above), most likely the reason why up to 60% While early or 24-h bond strength is mostly measured, there
of current scientific papers reporting on bond strengths have is a definite need to test bonding effectiveness of adhesives
employed the ␮TBS approach [41,42]. under more clinically relevant circumstances or upon aging
of the specimens. Indeed, many currently available dental
2.4. Micro-shear adhesives have presented with a relatively high short-term
bond strength, while not always equally favorable clinical
Also in order to generate as much specimens as possible results have been obtained. Therefore, more laboratory effort
from a single tooth, a micro-shear bond-strength test (␮SBS) should definitely go to durability testing of adhesion, rather
was introduced in 2002 [69,70]. This test combines the ease than measuring the ‘immediate’ bond strength. In up to
of manipulation with the ability to test several specimens 35% of the bond-strength studies, some kind of ‘aging’ fac-
per tooth. The very fine composite build-up (cylinder) with tor is added to the study design [41,42]. Water storage and
a typical diameter of 0.7 mm, in combination with a rela- thermo-cycling are the most popular artificial aging meth-
tive thick adhesive layer, may however result in considerable ods, but also other methodologies as mechanical loading and
bending and variable and non-uniform loading conditions. degradation by enzymes and various chemical substances
This non-uniform stress distribution is probably even more have been employed in literature [3]. Actually, the probably
pronounced as compared to macro-shear bond testing. Fur- most widely used aging technique is simple thermo-cycling,
thermore, it is impossible to confine the adhesive to the area although not always sufficiently long. A short thermo-cycling
tested, as required by ISO-standard No. 11405 (2003) [44]. Basi- regimen of 500 cycles, as recommended by the ISO TR 11450
cally due to these major shortcomings, this ␮SBS test has not standard (2003) [44], is of little use, while sometimes only
been adopted very well, since only 7% of recent bond-strength very long thermo-cycling up to 100,000 cycles can discrimi-
studies have used this protocol [41,42]. In a recent study com- nate differences in bond durability of different adhesives [86].
paring both MICRO-bond methodologies, it was shown that A well-validated method to assess bond durability is how-
the micro-shear values were about 1/3 of the micro-tensile ever the storage of micro-specimens in water [87]. Doing so,
values, while no difference in failure analysis was observed it was reported that within about 3 months, all classes of
[71]. adhesives exhibited mechanical and morphological evidence
of degradation that resembles in vivo aging [88]. Today, the
2.5. Fatigue current challenge in adhesive dentistry is indeed to make the
adhesive–tooth interface more resistant against aging, thereby
Besides static bond-strength tests, theoretically clinically rendering the restorative treatment more predictable in terms
more relevant is to test adhesive interfaces dynamically, as of clinical performance on the long term. The longevity of
in the clinical situation tooth-composite bonds are seldom bonded restorations is to a large extent related to the degrada-
subjected to acute tensile/shear stresses. It is rather exposed tion of the adhesive interface, which may occur in a relatively
to cyclic sub-critical loadings produced during chewing [3]. short term, depending on the way the adhesive has been
However, since such fatigue tests are even more labor- manipulated, on the actual adhesive approach and on the
intensive and time-consuming than static bond-strength adhesive composition. Hydrolysis of interface components,
tests, a steadily growing, but still only low number of fatigue such as dentinal collagen and resin, due to water sorption,
tests have been tried out throughout recent years on their potentially enhanced by enzymatic degradation, and sub-
potential to predict clinical effectiveness. In literature, 6 dif- sequent elution of the break-down products are the major
ferent fatigue tests have been reported on, as there are, factors lately identified as involved in this bond degradation
chronologically, (1) a macro-push-out fatigue test [53,54,72], process [3,4,10,26,30,89–91]. In fact, none of the current adhe-
(2) a macro-shear fatigue test [53,72–77], (3) a micro-rotary sives or techniques is today able to produce an interface that
fatigue test [78–80], (4) a micro-shear fatigue test [81], (5) is absolutely resistant to degradation, but fortunately many
a micro-4-point-bend fatigue test [82,83] and most recent research efforts are currently devoted to improving bond dura-
(6) a micro-tensile fatigue test [84,85]. Despite the alleged bility.
e108 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

Fig. 8 – Figure illustrating the micro-rotary fatigue approach developed by De Munck et al. [78–80], thereby showing some
typical fatigue phenomena such as ‘beach marks’ at the fracture plane.

2.7. KULeuven systematic review on bond strength solely when a proper ‘gold-standard’ control is included. Also
following the systematic review [41,42], the bond strength
At Leuven, we have recently thoroughly reviewed the literature of (resin-modified) glass-ionomers is scarcely tested, which
using the search term ‘dentin bond strength’ in PubMed with a could be due to the well-known fact that they tend to fail
limitation to PubMed-registered papers published in the last 5 cohesively within the material itself, while the actual bond
years [41,42]. This search was done on 18/01/2009 and revealed strength to tooth tissue can hardly be determined. Among
1019 studies, of which at the time of this paper 744 papers were the individual adhesives tested, the 2-step self-etch adhe-
evaluated on the following inclusion criteria: (a) measuring sive Clearfil SE Bond (Kuraray) was tested most (250 times),
bond strength to dentin; (b) involving at least two commercial followed closely by the 2-step etch&rinse adhesive Scotch-
adhesives; (c) only in combination with light-cure composites bond 1/Single Bond (3M ESPE) that was tested 211 times.
(no glass-ionomers, nor resin cements for instance); (d) and All other adhesives were substantially less frequently tested,
reporting at least the type of bond-strength test, the mean among which the 1-step adhesive Adper Prompt L-Pop (3M
bond strength in MPa, the standard deviation and the total ESPE) was tested 76 times, the 1-step adhesive Clearfil S3
number of specimens tested. So far, 214 studies were included Bond (Kuraray) 73 times, the 1-step adhesive One-up Bond
in the dataset, leading to 1828 bond-strength data for spe- F (Tokuyama, Tokyo, Japan) 62 times, the 2-step etch&rinse
cific adhesive/composite combinations. Most popular tests adhesive One-Step (Bisco, Schaumburg, IL, USA) 56 times, the
conducted were the micro-tensile bond-strength tests (1012 2-step etch&rinse adhesive Prime&Bond NT (Dentsply, Kon-
individual test groups were inserted in the database), followed stanz, Germany) 52 times, the 3-step etch&rinse adhesive
by macro-shear (287), micro-shear (221), and macro-tensile OptiBond FL (Kerr) 50 times, etc. From this dataset, already
(113) bond-strength tests. Only 26 macro-push-out and 12 some preliminary conclusions can be drawn. At first, there
micro-push-out bond-strength tests were reported on. Clearly, is an excessive number of bond-strength data published in
the most recent 1-step adhesives were tested most frequently literature and the variability between the studies is huge.
(531), followed closely by both the 2-step etch&rinse (510) Especially the difference between the different test set-ups is
and 2-step self-etch adhesives (450), while somewhat surpris- remarkable; a simple general linear model revealed that the
ingly the traditional 3-step etch&rinse adhesives have been weighted mean of all micro-tensile bond-strength values is
tested least frequently (173). This finding confirms that still too about twice as high as the weighted mean of the macro-shear
often in many of today’s bond-strength studies so-called ‘gold- test (16 versus 30 MPa). As the fine details of the bond-strength
standard’ controls, by preference a well-documented and test in the first place determine the height of the absolute
consistently good-performing 3-step etch&rinse or 2-step self- bond strength, it therefore does make not much sense to state
etch adhesive, are lacking in the study set-ups. Perhaps should that a certain absolute value in MPa is needed for a product to
journals be more strict in publishing bond-strength studies be clinically effective. Likewise, striving for a standard bond-
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e109

one should not underestimate the perhaps higher technique-


sensitivity involved in fracture mechanics, by which also using
this methodology large scattering of the data among the
diverse research centers worldwide can hardly be avoided.

3. Assessment of sealing ability

As the longevity of an adhesive composite restoration is


mainly affected by leakage of oral fluids along the interface
between restorative material and tooth substrate [104,105],
probably more clinically relevant than bond-strength stud-
ies is to evaluate the capacity of an adhesive to maintain
Fig. 9 – Upon the systematic review recently conducted on the tooth-restoration transition sealed. It is especially thought
bond strength at Leuven [41,42], the weighted to predict better the clinical performance of adhesives with
bond-strength means were found to clearly differ per regard to the occurrence of postoperative sensitivity and/or
adhesive class. The weighted mean and large confidence secondary caries [105].
interval for the (2-step) glass-ionomers is less trustworthy,
since only few products could be included at the moment 3.1. Micro-leakage
this paper was written.
Leakage on the micrometer scale (micro-leakage) is often
assessed in vitro microscopically on cross-sections using a
strength test, enabling bond strength to be measured as a wide variety of tracers or dyes that are able to infiltrate
true material property (thus independent from the test set-up, the composite–tooth interface, such as silver nitrate, methy-
and reproducible in different research institutes worldwide), lene blue, basic fuchsin, and erythrosine [104], and even
is most likely never achievable. Following the present sys- some radioactive markers [105]. Although such micro-leakage
tematic review [41,42], significant differences in the ‘pooled’ assessment is in principle even easier than bond-strength
mean bond strength can be observed, as the weighted bond- measurements (and therefore done very frequently), the
strength means of individual adhesives ranges from about reliability of conventional micro-leakage protocols remains
12 MPa (for Absolute, Dentsply-Sankin, Tokyo, Japan) to 49 MPa controversial [104,106,107]. Like for bond-strength studies,
(for OptiBond FL, Kerr) and the weighted bond-strength means a systematic review of dye penetration studies for restora-
per adhesive class range from 31 MPa for 3-step etch&rinse tive materials concluded that a comparison of study results
adhesives, to 29 MPa for 2-step self-etch adhesives, 26 MPa for is impossible due to the great variability of methodol-
2-step etch&rinse adhesives, and 20 MPa for 1-step self-etch ogy parameters employed worldwide [104]. In addition, the
adhesives (Fig. 9). The weighted mean and large confidence cross-section-based procedure is destructive and part of the
interval for the 2-step glass-ionomers is less trustworthy since specimen is lost through slicing. More importantly, the pro-
only few products could be included at the moment this paper cedure allows only a limited 2D-view on the distribution of
was written. the marker fluid, by which it is for instance not possible to
determine the point of deepest leakage with certainty. Newer
2.8. Fracture mechanics so-called micro-permeability tests make use of fluorescent
dyes like rhodamine, that are ‘loaded’ to the pulp chamber
As concluded in the ADM review paper from Scherrer et al. in order to investigate at higher resolution using confocal
[92], the high scatter in dentin bond-strength data found in microscopy the sealing ability of adhesives at the interface
the literature, regardless which current bond-strength test is itself [108–110].
used, should be attributed primarily to non-uniform stress dis-
tributions due to a number of geometrical, loading, material 3.2. Marginal adaptation/gap formation
property and specimen-preparation variables, as this was also
confirmed by Finite Element Analysis [45,47,48,59,60,93,94]. Another technique to assess marginal sealing ability involves
It has been proposed that an interfacial fracture mechanics a semi-quantitative marginal analysis of replicas of restored
approach that studies the failure of an interface by the initi- teeth using SEM, combined with custom-made software
ation and growth of a single, large, dominant crack, such as to measure the length of the margin part that exhibits a
the fracture toughness test, would be more appropriate for (gap-free) ‘continuous margin’ versus any kind of marginal
testing the relatively brittle adhesive–tooth interface [92,95]. defect following a pre-determined set of margin qualities
Nevertheless, this fracture mechanics approach has so far [106,111,112]. Besides being laborious and time-consuming
not received much support despite several fracture toughness (most likely being the main reasons why this methodology
measurements of adhesives have previously been reported on is solely consistently used in a few research centers), another
[96–103]. Probably, the big hurdle to take is the more labori- major drawback of this technique is that it only enables to
ous and time-consuming specimen preparation, by which this assess marginal sealing in 2D at the outer surface. The advan-
methodology no longer meets with the basic requirements of tage of using replica’s however is that the same margins can
an easy and fast, and ‘first’ product-screening test. In addition, be assessed multiple times after having exposed the spec-
e110 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

imens to some kind of aging procedure [112]. A simplified clinical effectiveness of a restorative treatment [2,6,141,142].
marginal sealing screening test evaluates the gap formation The popularity of in vitro studies in the field of adhesive den-
around standardized cylindrical cavities, a test introduced tistry may in part be ascribed to the rapid evolution of dental
a long time ago [106,113]. Based on this simple approach, adhesive technology and the resultant high turnover of adhe-
an automated system has recently been developed that can sive systems, which often tempts manufacturers to release a
detect marginal gaps automatically using an optical sensor successor product on the market even before its precursor has
[114]. Using this automated methodology, 21 adhesives were been clinically evaluated, at least on the long term. By carrying
for instance screened on their ability to produce gap-free out in vivo studies, all possible aging factors play at the same
margins [115]. This study revealed that the etch&rinse adhe- time, thereby disclosing whether an adhesive is truly reliable
sives demonstrated the best marginal adaptation, followed for routine clinical practice.
by the 2-step self-etch adhesives. The 1-step self-etch adhe-
sives yielded the poorest marginal adaptation and the highest 4.1. Class-V clinical data
scatter in test results between materials and within the same
material. Clinical effectiveness of adhesives should best be determined
using Class-V clinical trials, because (1) such lesions do not
3.3. Bacterial leakage provide any macro-mechanical retention, so that ineffective
bonding will result in early restoration loss, (2) Class-V restora-
A bacterial micro-leakage model has mainly been applied in tion margins are located in enamel as well as in dentin,
endodontic research [116–119]. (3) lesions are commonly located on vestibular surfaces of
anterior teeth and premolars, thus providing good access
3.4. Permeability for the restorative procedure as well as evaluation (visually
using an explorer and magnifying glasses, and even by SEM
A full-quantitative test to measure sealing ability has been if epoxy replicas are made), (4) preparation and restoration
developed on basis of the early dentin permeability studies of Class-V lesions is minimal and relatively easy, thereby
by Reeder and Pashley et al. [120–123], but is perhaps too somewhat reducing practitioner variability, (5) lesions are rel-
technique-sensitive to become a standard test to screen adhe- atively wide spread and prevail on multiple teeth, facilitating
sives on their sealing ability [124,56]. patient selection and enabling split-mouth study designs, and
(6) Class-V lesions have a relatively small C-factor, by which
3.5. Nano-leakage the mechanical properties of the composite used are more
or less unimportant and the actual adhesive performance
Just like ‘classical’ micro-leakage assessment, also qual- determines the eventual clinical outcome to a great extent
itative imaging and certainly quantification of so-called [2,6,142–145]. Retention, marginal integrity and clinical micro-
nano-leakage (as per definition being ‘the diffusion of small leakage are usually the key parameters recorded to judge
ions or molecules within the hybrid layer in the absence upon clinical effectiveness of adhesives. Definitely the most
of gap formation’ [125,126]), using SEM, TEM or confocal objective criterion is retention, by which Class-V clinical data
microscopy [127–130] should also be interpreted with care recorded worldwide can be mutually compared [2].
[131]. The high regional variability makes it very difficult to At KULeuven (Belgium), there is a long track record in con-
obtain representative information with regard to the resis- ducting Class-V clinical trials [2,6,141,142,145–158], as part of
tance of adhesives against nano-leakage. Moreover, at least our overall translational research line within BIOMAT on the
5 independent studies agree on the absence of any correla- development of new adhesive dental restorative materials.
tion between nano-leakage and bond strength of adhesives This research line involves basic research investigating molec-
[132–135]. ular interactions of functional monomers with inorganic tooth
tissue components, applied research up to mechanical testing
3.6. 3D-leakage of adhesive interfaces, and eventually clinical research into
the ultimate clinical performance of new adhesive materi-
For leakage, either micro- or nano-leakage, to be a valuable als/procedures in the mouth of patients (KULeuven University
criterion for evaluating adhesive performance, a fully quan- Hospital). From the start in the mid-1980s, almost the same
titative methodology that measures leakage in three rather standard study design has been employed. The data collec-
than two dimensions is most likely required [131]. In search tion was done by well-trained and calibrated examiners in an
for a full-quantitative 3D leakage test, microfocus-CT with a attempt to maintain the study quality equally high, basically
potential resolution of the order of 1 ␮m (depending on the enabling the Class-V data that have been collected throughout
hardware capabilities and X-ray source characteristics) has the past 25 years be compared mutually. The major outcome
recently been tried out [132–140]. strived for was always the basic clinical effectiveness of exper-
imental and/or commercial adhesives, while sufficient care
was taken to include an appropriate control(s) within each
4. Clinical performance individual study. The major modifications of the initial clinical
trial protocol to the current one entail a gradually increas-
Despite the importance of laboratory studies attempting to ing number of restorations/patients (a), as well as a shift of a
predict clinical performance of biomaterials, clinical trials ‘split-mouth’ design to a ‘pair-tooth’ study design (b). We cur-
remain the ultimate way to collect scientific evidence on the rently place at least 50 Class-V restorations per experimental
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e111

Fig. 11 – Graph representing the retention rate of Class-V


Fig. 10 – Graph representing the retention rate of Class-V restorations up to 8 years of clinical service for a 2-step
restorations up to 13 years of clinical service for three self-etch adhesive with and without selective phosphoric
3-step etch&rinse adhesives [156,161]. This study is acid etching of enamel [157,165]. This study is conducted at
conducted at the Catholic University of Leuven in Belgium the Catholic University of Leuven in Belgium (KULeuven).
(KULeuven). Be aware that the retention rate (in the Y-axis) Be aware that the retention rate (in the Y-axis) starts at 50%.
starts at 75%.

effectiveness of two 3-step etch&rinse adhesives in combi-


nation with a hybrid, stiffer composite versus a micro-filled,
group in at least 50 patients, by which we comply with the
more flexible composite (Fig. 10) [156,161]. After 13 years of
current recommendations for conducting randomized con-
clinical service, 94% of the restorations in the control group
trolled clinical trials (RCT) of dental restorative materials [159].
(OptiBond FL in combination with Prodigy, Kerr) were still in
(a) Although in the latter recommendations it is stated that
function. After this long clinical service, obviously marginal
the clinical investigator performs only two restorations per
defects and discolorations were observed at a steadily grow-
patient (one restoration per experimental group), we believe
ing incidence, but most are only minor defects that do not
that it is of primary importance to include a sufficiently
require urgent restoration repair and certainly not restoration
high number of restorations in the clinical trial. We therefore
replacement. As flexure at the tooth cervix has been advanced
nowadays employ a ‘multi-restoration approach’, by which we
as one of the three principal factors causing non-carious cer-
restore ALL Class-V lesions that need to be restored within one
vical lesions [162,163], it was reasonable to hypothesize that
patient, equally dividing ad random the lesions per experimen-
tal group. It is of course correct that treating more than one
lesion per condition within one mouth introduces a potential
‘patient factor’ (dependent data), but this does not necessar-
ily mean that the power of the study cannot be increased by
this multi-restoration approach. Provided that a suitable (but
unfortunately more complex) statistical analysis is applied,
the supplementary restorations may still add new informa-
tion. The eventual increase in power of the study will depend
on the strength of correlation between the repeated measure-
ments (within one patient). Only in the worst case, when the
clinical outcome is completely determined by patient factors,
one can return to a one-restoration-per-condition-per-patient
analysis by ad random (and multiple times) selecting pairs of
restorations within each mouth. Most often, the patient factor
will have some influence, but will never completely determine
the outcome so that treating more lesions per patient with the
same material (as patients often present with multiple Class-
V lesions) is an easy and valid option to prevent conducting Fig. 12 – Graph representing the retention rate of Class-V
clinical trials with low sample size and thus power [160]. (b) restorations up to 3 years of clinical service for two 1-step
The second ‘pair-tooth’ design indicates that restorations will self-etch adhesives as compared to that of a 3-step
always be placed in pairs of two restorations (each experimen- etch&rinse control adhesive [158,166,167]. This study is
tal group) in nearly equal teeth (first and second premolar at conducted at three university institutes, namely the
the same side, left and corresponding right incisor, canine or University of Sao Paulo in Brazil (USP), the Suleyman
premolar, respectively). Demirel University at Turkey (SDU), and the Catholic
At the moment, we run three Class-V studies at Leuven University of Leuven in Belgium (KUL). Be aware that the
(Figs. 10–12). (KUL-1) A long-term study evaluates the clinical retention rate (in the Y-axis) starts at 50%.
e112 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

similar stress is imposed to restored Class-V lesions, thereby OptiBond Solo, Kerr; Prime&Bond NT, Dentsply; Single Bond,
promoting marginal degradation or even dislodgement of the 3M ESPE), 1-step (self-etch) adhesives (Adper Prompt LP-2, 3M
restoration [150,164]. This study however failed to prove that ESPE; iBond, Hereaus-Kulzer; One-up Bond, Tokuyama; Vari-
the composite stiffness affects the clinical longevity of cervical glass, Dentsply), and (resin-modified) glass-ionomers (Fuji II
composite restorations. (KUL-2) In a second long-term study, LC, GC; Variglass, Dentsply), have been evaluated in non-
the clinical effectiveness of a ‘mild’ 2-step self-etch adhesive carious Class-V lesions in a consistent way (Fig. 13) [169–176].
(Clearfil SE Bond) was evaluated (Fig. 11) [157,165]. At 8 years, For the 3-step etch&rinse adhesive, OptiBond Dual Cure (Kerr),
the clinical effectiveness appeared excellent, with selective 12-year data are available, reporting a very high retention rate
acid-etching of the enamel margins only having some minor of 93% [175]. While almost all other retention curves show
effect on secondary clinical parameters (higher incidence of a clear downward trend, that of OptiBond Dual Cure (Kerr)
small marginal defects/discolorations at enamel that were of remains high and rather stable on a long-term perspective.
clinical negligible relevance, since they did not require any Especially the difference with its 2-step etch&rinse successor
restorative intervention at the 8-year recall). (KUL-3) The most (OptiBond Solo, Kerr) is striking, as for this adhesive after 8
recent clinical Class-V study is multi-center based and evalu- years the retention rate dropped to 69% [176]. Likewise, the
ates the clinical performance of two 1-step self-etch adhesives 8-year retention rate of the acetone-based 2-step etch&rinse
(G-Bond, GC; Clearfil S3 Bond, Kuraray) in comparison to adhesive, Prime&Bond 2.1 (Dentsply), dropped to even 59%
the ‘gold-standard’ 3-step etch&rinse adhesive (OptiBond FL, [176]. Also the water-based 3-step and 2-step etch&rinse adhe-
Kerr) (Fig. 12) [158,166,167]. Each of the studies did exam- sives Scotchbond MP and Single bond (both from 3M ESPE)
ine two adhesives following the same multi-restoration and performed rather equally with retention rates of, respectively,
paired-tooth design explained above. Up to 2 years of clinical 78% and 75% at 3 years [172]. They both however cannot
service, no major differences in clinical performance between compete with the ethanol-based 3-step etch&rinse adhesive
the 1-step adhesives and the 3-step etch&rinse control were OptiBond Dual Cure (Kerr), being the precursor of the still cur-
observed. Obviously, longer-term clinical evaluation is needed rently commercially available successor OptiBond FL (Kerr).
in respect to bond durability. In a recent Class-V clinical trial by Regarding the clinical performance of 1-step adhesives, it is
Burrow and Tyas [168], a 3-year retention rate of, respectively, worth to mention the steep drop in retention rate of Adper
100% and 97% was recorded for the 1-step adhesives G-Bond Prompt LP-2 (3M ESPE) to 81% at 1.5 years of clinical service
(GC, in combination with the composite Gradia, GC) and for [172], while for the more recently marketed ‘mild’ 1-step self-
Clearfil S3 Bond (Kuraray, in combination with the composite etch adhesives, iBond (Hereaus-Kulzer), so far no losses were
Clearfil ST, Kuraray). recorded (100% retention rate at 1.5 years) [174], and for One-
At UNC (USA), a wide spectrum of adhesives, among up Bond (Tokuyama) a less favorable retention rate of 90% was
which 3-step etch&rinse adhesives (OptiBond Dual cure, Kerr; recorded [173].
ProBond, Dentsply; Scotchbond MP, 3M-ESPE; Gluma Solid Two other long-term Class-V studies worth mentioning
Bond, Hereaus-Kulzer, Hanua, Germany), 2-step etch&rinse were performed at Umeå University (Sweden) by Van Dijken
adhesives (Excite, Ivoclar-Vivadent, Schaan, Liechtenstein; et al. (Fig. 14) [177,178]. At Umeå, the retention rates of Class-V

Fig. 13 – Graph representing the retention rate of Class-V restorations up to 12 years of clinical service for 13 different
commercial adhesives (Single Bond (3M ESPE) was tested twice). These studies are (have been) conducted at the University
of North Carolina at Chapel Hill (UNC) [168–175]. Be aware that the retention rate (in the Y-axis) starts at 50%.
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e113

the last decade. As at Umeå recalls have systematically been


done on a year basis, the data clearly show the continuous
degradation in bonding effectiveness of all adhesives tested,
though at a significantly varying speed for each individual
adhesive. Again, if enamel would have been bonded to as well,
the retention data would obviously have been much higher.
This once again confirms that bonding to dentin remains very
challenging, in the laboratory as well as clinically. Some more
recent Class-V retention rates of studies conducted at Umeå
University are mentioned in Fig. 14 [179]. They again confirm
the improved clinical effectiveness of recent-generation adhe-
sives, even when applied in less application steps.
Considering only the really long-term clinical data, not
much information on long-term clinical effectiveness of adhe-
sives is today available, especially when abstracting the Umeå
data because of the dentin-only study design. The most favor-
Fig. 14 – Graph representing the retention rate of Class-V able long-term (retention) data have been recorded for the
restorations up to 13 years of clinical service for 13 different 3-step etch&rinse adhesives Optibond FL (Kerr) and its precur-
commercial adhesives. These studies have been conducted sor Optibond Dual-Cure (Kerr). At Leuven, Optibond FL (Kerr)
at Umeå University (Sweden) [176,177]. Some recent clinical presented with a 94% retention rate at 13 years [161], while
retention rates [178] are depicted by letters in the graph. For even a 97% retention rate was recorded at Chicago [180]. At
the 3-step etch&rinse adhesive cmf (‘a’: Saremco; in Chapel Hill, an almost equally high retention rate of 93% was
combination with the composite els, Saremco), a 1.5-year recorded for OptiBond Dual Cure (Kerr) at 12 years [175]. The
retention rate of 96% was recorded versus a 1.5-year only other favorable retention rate (97%) was recorded for the
retention rate of 91.8% for the 2-step etch&rinse adhesive 2-step self-etch adhesive Clearfil SE Bond (Kuraray) at 8 years
XP-Bond (‘b’: Dentsply; also in combination with the [157,165].
composite els, Saremco). For the 2-step self-etch adhesive
Clearfil Protect Bond (Kuraray), a 1.5-year retention rate of 4.2. KULeuven systematic review on Class-V clinical
98.2% was recorded when used in combination with both data, Part I
the composite Tetric Ceram (‘c’: Ivoclar-Vivadent) and els
(‘d’: Saremco). A 3-year retention rate of, respectively, In an attempt to get a better insight in the current over-
96.7%, 96.5% and 93.7% have been recorded at Umeå all clinical performance of adhesives, we refer to a relatively
University for G-Bond (GC), AdheSE (Ivoclar-Vivadent) and recently conducted systematic review, in which the annual
Clearfil SE Bond (Kuraray). failure rates were determined per adhesive class (Fig. 15)
[2]. According to that review, the best clinical performance
with regard to retention has so far been achieved by glass-
ionomers. Their low annual failure rates can be ascribed to
restorations placed using 13 different adhesives were sys- their unique self-adhesiveness, based on the twofold micro-
tematically recalled up to 13 years of clinical service. For mechanical and chemical bonding mechanism (see above).
correct interpretation of the Umeå data, it is important to Despite their excellent clinical performance in terms of reten-
mention that all restorations were placed in dentin lesions
without any intentional enamel involvement. In this respect,
only the clinical bonding performance to dentin was evalu-
ated, in contrary to most other (also the above-mentioned)
Class-V studies, in which the adhesive was applied to both
enamel and dentin in a so-called mixed enamel/dentin lesion.
After 13 years, only 5 adhesives presented with a retention
rate higher than 50%: the 3-step etch&rinse adhesive Clearfil
Liner Bond (Kuraray) with 74%; the 3-step etch&rinse adhe-
sive OptiBond Dual Cure (Kerr) with 59%; the resin-modified
glass-ionomer Vitremer (3M ESPE) with 64%; the 2-step self-
etch adhesive ART Bond (Coltène, Altstätten, Switzerland)
with 59% and the 3-step etch&rinse adhesive Syntac Classic
(Ivoclar-Vivadent) with 64%. The four worst-performing adhe-
sives (retention rates below 30% at 13 years) were all obsolete
adhesives that fortunately are no longer commercially avail-
able. The clinical bonding performance of the more recently Fig. 15 – Graph representing the mean annual failure rates
marketed adhesives is clearly better, corresponding to the bet- per adhesive class, determined according to a systematic
ter laboratory data reported on in literature and thus with the review of Class-V clinical trials of adhesives during the
great progress dental adhesive technology has undergone in period 1998–2004 [2].
e114 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

tion, glass-ionomers commonly present with lower aesthetic


features when compared to resin-based restorative materi-
als. The poorer mechanical properties of glass-ionomers also
explain the lower scores achieved in bond-strength tests when
compared to those of resin-based adhesives, by which a glass-
ionomer typically fails cohesively rather than it de-bonds
from the tooth surface (see above). Besides glass-ionomers,
in particular 3-step etch&rinse adhesives have exhibited a
reasonably good clinical effectiveness (Fig. 15) [2]. The clin-
ical durability of 3-step etch&rinse adhesives confirms their
generally superior laboratory results, in which they are con-
sidered as ‘gold-standard’ and often employed as control
to compare the performance of new-generation adhesives
with. According to the same standard, 2-step self-etch adhe-
sives tend to approach the clinical performance of 3-step
etch&rinse adhesives in terms of low annual failure rates Fig. 16 – Graph representing the mean annual failure rates
(Fig. 15) [2]. Their ability to provide a shallow but uniform per adhesive class, determined according to a systematic
hybrid layer, along with their capability to chemically bond review of Class-V clinical trials of adhesives during the
to the dentin substrate seems to play an important role to period 2004–2009 [182], in continuation of the earlier con-
resist long-term hydrolytic degradation (see above). Com- ducted review during the period 1998–2004 [2]. The overall
monly, the clinical performance of such self-etch adhesives mean annual failure rates per adhesive class for the total
does not vary substantially from one study to another, which 10-year review period (1998–2009) are mentioned as well.
is indicative of their rather low technique-sensitivity. Further-
more, another clinically important benefit is, as mentioned
before, that these self-etch adhesives are repeatedly associ- adhesives. This is not that surprising taking into account
ated with very low levels of postoperative sensitivity [181]. that these self-etch adhesives make use of a bonding mech-
In general, 2-step etch&rinse adhesives have performed less anism that most closely approaches that of glass-ionomers
favorably than the conventional 3-step version (Fig. 15) [2]. (see above). Including all 2-step self-etch adhesives (also the
Laboratory studies have corroborated these results, ascribing so-called ‘strong’ self-etch adhesives) substantially increases
their poorer performance to their higher hydrophilicity and the annual failure rates. This can also be explained as these
reduced hybridization potential (see above). It is noteworthy ‘strong’ self-etch adhesives significantly performed worse in
that irrespective of the number of application steps, acetone- laboratory, especially regarding their bonding efficiency to
based etch&rinse adhesives have generally performed less dentin. As mentioned above, the aggressive self-etch proce-
satisfactorily than their water/ethanol-based alternatives. The dure of these ‘strong’ self-etch adhesives relatively deeply
above-mentioned high technique-sensitivity of acetone-based dissolves HAp (exposing collagen). As these adhesive do not
adhesives must be the reason for their compromised long- involve a rinse step, the dissolved calcium phosphates are
term clinical data. According to this review [2], a so far embedded within the hybrid layer. These calcium phosphates
rather inefficient clinical performance has been noted for are however not very hydrolytically stable, thereby seriously
the newest generation of 1-step adhesives. Widely varying jeopardizing the bond longevity. Somewhat higher annual fail-
retention scores have been recorded, indicating their high ure rates were recorded for the 3-step etch&rinse adhesives,
technique-sensitivity despite their user-friendliness (Fig. 15). but they decreased in the more recent literature review, also
Such lower bonding performance must be ascribed to the having resulted in a decreased annual failure rate for the
many concerns advanced earlier. whole 10-year review period (1998–2009). The annual failure
rate of the 2-step etch&rinse adhesives remained nearly sta-
4.3. KULeuven systematic review on Class-V clinical ble, while that of the most simple-to-use 1-step adhesives
data, Part II substantially improved in the most recent literature, even to
an annual failure rate in line with that recorded for the 3-
On the occasion of this manuscript and the ADM 2009 meet- step etch&rinse adhesives in the same period. For the whole
ing at Portland, the systematic review of the literature that 10-year review period, the annual failure rate of the 3-step
appeared in the period 1998 until 2004 [2], was continued in etch&rinse adhesives is still significantly lower. Nevertheless,
the same way for the literature that appeared in the period it is noteworthy that the most recent generation of 1-step
2004–2009 and has provided new data with regard to annual adhesives have substantially improved and evolve definitely
failure rates per adhesive class [182,183] (Fig. 16). Besides the in the good direction (Fig. 16).
calculation of the annual failure rates per adhesive class for
the new period 2004–2009, also both datasets were combined,
revealing annual failure rates for the 10-year period 1998–2009. 5. Relationship between laboratory and
Still the lowest annual failure rates have been recorded for the clinical bonding effectiveness
glass-ionomers, irrespective of the time period during which
the literature was reviewed. Equally favorably performed the The ultimate question is if there is a relationship between
so-called ‘mild’ and ‘intermediately strong’ 2-step self-etch the bonding effectiveness measured in the laboratory with
d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121 e115

the clinical effectiveness determined in patients. In other 5.3. Relationship III


words, can we predict clinical effectiveness in the laboratory?
Although it is hard to give a straightforward answer to this In a more recent study by Heintze et al. [185], a correlation
question, there are some trends that certainly point to cer- analysis was performed between micro-tensile bond-strength
tain associations between laboratory and clinical data on the data and the same clinical index. Again, no significant correla-
bonding effectiveness of adhesives. tion could be found between the micro-tensile bond-strength
data and the clinical index, nor with the clinical retention
rate and marginal integrity. The only significant correlation
5.1. Relationship I
found existed between micro-tensile bond strength, espe-
cially measured after 6-month water storage, and the marginal
A good correlation coefficient of 0.81 was found between
discoloration of Class-V restorations. The authors therefore
the annual failure rates reported in the systematic review of
suggested that early marginal staining could be predictive for
Peumans et al. [2] and the ‘Battle-of-the-Bonds’ shear bond-
future retention loss of non-carious cervical restorations. One
strength data from Degrange et al. [49,50].
should however keep in mind that the clinical evaluation of
marginal staining is rather subjective, and may lead to sub-
5.2. Relationship II stantially more variance in data when considered worldwide.

In a study by Heintze et al. [184], searching for a correlation 5.4. Relationship IV


between semi-quantitative margin analysis data (see above),
as performed in two research centers, and a somewhat arti- On the occasion of this manuscript and the ADM 2009
ficial clinical index, consisting of retention loss, marginal meeting at Portland, we have searched for a potential rela-
discoloration, and marginal integrity (weighted), only a weak tionship of the laboratory bond-strength data obtained in
correlation was found. The in vitro measured ‘marginal adap- the recently performed systematic review [41,42], with the
tation’ appeared to only have a mediocre value in terms of clinical retention rates collected in the systematic review
its ability to predict the clinical performance of adhesives (in on the clinical effectiveness of adhesives in Class-V lesions
cervical cavities). Unfortunately, the analysis was hampered (Fig. 17) [2,182,183]. For this analysis, the complete database
by the great variability in clinical results, but also by the fact (bond strength – all) was used, but also a database filtered
that no correlation was found between the in vitro methods for bond-strength data measured after the specimens had
employed at both research institutes involved. been subjected to some kind of in vitro aging procedure (bond

Fig. 17 – Correlation analysis between bond-strength data [41,42] and clinical Class-V retention rates [2,182]. Bond-strength
data were extracted and a weighted mean was calculated, considering all data in the database (bond strength – all), or only
for those data that were recorded after the specimens were subjected to some kind of durability factor (as for example water
storage, thermo-cycling, etc.) (bond strength – durability). For the clinical data, retention rates after 2 years (Class-V
retention rate at 2 years) as well as after 5 years of clinical service (Class-V retention rate at 5 years) were gathered.
Correlation analysis revealed that the bond strength seems not to predict the 2-year clinical outcome (no significant
correlation). The bond-strength data gathered after in vitro aging appear more clinically relevant and do predict the clinical
performance on the longer term (5 years) to some extent (r = 0.5811, p = 0.0475).
e116 d e n t a l m a t e r i a l s 2 6 ( 2 0 1 0 ) e100–e121

strength – durability). Regarding the clinical data, the reten- ferent cocktails of adhesive solutions to enamel and dentin in
tion rate at 2 years was first chosen (Class-V retention rate the laboratory. The adhesive formulation that scores best com-
at 2 years), as this was the point in time when most reten- monly makes it rapidly to the market, after which the superior
tion rates were available. In a second phase, also the retention laboratory performance of the product is hopefully confirmed
rate at 5 years was used (Class-V retention rate at 5 years), in independent randomized controlled clinical trials. Much
which is the longest recall time that still revealed sufficient knowledge on the underlying mechanisms of adhesion to
data. Using these criteria, the preliminary correlation anal- enamel and dentin has been gathered by numerously imag-
ysis did not reveal any significant correlation between both ing adhesive–tooth interfaces with all sorts of microscopes.
parameters for the 2-year clinical data and the 5-year clini- On the contrary, the actual molecular interactions at the inter-
cal data, the latter correlated to the complete bond-strength face have hardly been explored. Also many basic questions
dataset (Fig. 17). A significant, quite reasonable correlation was still remain unanswered, like for instance why certain func-
nevertheless found between the aged bond-strength data and tional monomers have better bonding potential than others,
the 5-year clinical data. The fact that no one-to-one relation- and why mild self-etch adhesives with additional chemical
ship between the in vitro and in vivo 2-year data exists, should bonding do not perform better at enamel. Thus, fundamen-
be attributed to the fact that many adhesives then still show tal for future design and development of dental adhesives
a very high retention rate (about half of the studies revealed is the further unravelling of the interfacial molecular
retention rates higher than 95% at 2 years). Another plausible interactions.
reason is that regarding the aged bond-strength data no cor- Finally, the ultimate objective of this paper (and presen-
rection was for instance performed for the kind of aging. So, a tation) was to search for a potential relationship between
regime of 500 thermo-cycles was for example pooled with 1- laboratory bond-strength data and clinical outcomes. After an
year water-storage data, although the latter aging procedure extensive discussion of the different laboratory test method-
should have resulted for sure in more bond degradation than ologies to measure bond strength (and sealing ability), and
the former. On the other hand, as could be expected from the presentation of the most recent clinical effectiveness
the longer-term 5-year clinical data, a trend for association data (with regard to retention rates of adhesive Class-V
between in vitro bond strength and the clinical data becomes restorations), some clear indications for correlation of labo-
apparent for the complete dataset, and even significant when ratory bond strength with clinical retention rates of Class-V
all non-aged bond-strength data were excluded. restorations have been advanced, in particular of ‘aged’
bond-strength data with medium-term retention rates. Con-
sequently, besides measuring the ‘immediate’ bond strength
6. Conclusions and closing remarks of adhesives to enamel and dentin, measuring the ‘aged’ bond
strength should be encouraged in order to predict the clinical
Adhesive technology has undergone great progress in the last effectiveness of adhesives.
decade. In light of the major drawbacks attributed to all-in-
one adhesives, conventional 3-step etch&rinse adhesives and
(mild) 2-step self-etch adhesives are still the benchmarks for Acknowledgments
dental adhesion in routine clinical practice. When bonding
to enamel, an etch&rinse approach is definitely preferred, The authors would like to thank Michael Burrow et al. (Univer-
indicating that simple micro-mechanical interaction appears sity of Melbourne), Ed Swift et al. (University of North-Carolina
sufficient to achieve a durable bond to enamel. When bonding at Chapel Hill), and Jan Van Dijken et al. (Umeå University) for
to dentin, a mild self-etch approach is superior, as it involves disclosing their most recent Class-V clinical data, and Sieg-
(like with glass-ionomers) additional ionic bonding with resid- ward Heintze et al. (Ivoclar-Vivadent) for sharing their most
ual HAp. This additional primary chemical bonding definitely recent laboratory and clinical correlation data.
contributes to bond durability. Altogether, when bonding to
both enamel and dentin, selective etching of enamel followed
by the application of the 2-step self-etch adhesive to both references
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