d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226

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The relationship between cyclic hygroscopic

dimensional changes and water
sorption/desorption of self-adhering and new
resin-matrix composites

Yong-jie Wei a,b , Nick Silikas b , Zhen-ting Zhang a,∗ , David C. Watts b,c,∗∗
a Department of Prosthodontics, School of Stomatology, Capital Medical University, Beijing, PR China
b Biomaterials Science Research Group, School of Dentistry and Photon Science Institute, The University of
Manchester, UK
c Institute of Materials Science and Technology, Friedrich Schiller University, Jena, Germany

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

Article history: Objectives. This study evaluated the relationship between mass changes and hygroscopic
Received 9 April 2012 dimensional changes during water sorption/desorption cycles in new resin composites.
Received in revised form Methods. A silorane posterior composite (Filtek® Silorane, FS), two micro-fine hybrid compos-
15 May 2013 ites (GC Gradia Direct Anterior, GDA; GC Gradia Direct Posterior, GDP), a universal composite
Accepted 23 May 2013 (GC Kalore, GCK), and a self-adhering flowable composite (Vertise® Flow, VF) were evalu-
ated. 25 (n = 5) disk specimens (15 mm × 2 mm) were prepared according to ISO 4049. Water
sorption was measured gravimetrically. Hygroscopic expansions were measured by a laser
Keywords: micrometer regularly during 150 d water storage and 40 d recondition periods, all at 37 ◦ C.
Resin composite Data were analyzed by repeated measures ANOVA, one-way ANOVA and Tukey’s post hoc test
Water sorption (p < 0.05).
Desorption Results. Mass changes after 150 d water immersion ranged from 0.68% (±0.02) for FS to
Hygroscopic expansion 2.83% (±0.11) for VF and the corresponding hygroscopic expansions were from 0.74% (±0.05)
GPDM for FS to 4.79% (±0.18) for VF. The differences were significant for all materials (p < 0.001),
Silorane except mass changes between GCK and GDP, as well as hygroscopic changes between GCK
DX-511 and GDA. The relationship between hygroscopic expansions and mass changes was ini-
UDMA tially non-linear and then tended toward linear behavior. But at the late stage of water
sorption the hygroscopic expansion of GCK and VF was slightly sigmoidal with respect to
their mass changes.
Significance. Relationships between hygroscopic expansion and mass change were deter-
mined for some diverse resin-matrix composites. The initial non-linearity for all materials

∗
Corresponding author at: Department of Prosthodontics, School of Stomatology, Capital Medical University, Tiantan Xili No. 4, Dongcheng
District, Beijing 100050, PR China. Tel.: +86 10 5701 2783; fax: +86 10 5701 3995.
∗∗
Corresponding author at: Biomaterials Science Research Group, School of Dentistry, The University of Manchester, Higher Cambridge
Street, Manchester M15 6FH, UK. Tel: +44 161 275 6749.
E-mail addresses: [email protected] (Y.-j. Wei), [email protected] (Z.-t. Zhang), [email protected] (D.C. Watts).
0109-5641/$ – see front matter © 2013 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.dental.2013.05.010
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226 e219

suggests a lower expansion rate due to occupancy of internal free volume by water ingress.
The silorane composite FS showed statistically the lowest mass change and hygroscopic
dimensional change.
© 2013 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.

and hygroscopic expansion for a set of six light-cured poste-

1. Introduction rior resin composites [18]. This poor correlation might due to
the diversity of materials. Also many differences in specimen
Esthetic restorations consisting of resin composites continu- size and shape were reported in different studies. Conse-
ously encounter a wet intra-oral environment. Thus, during quently, the relationship between hygroscopic dimensional
clinical service, these materials may experience water-related changes and mass uptake for some contemporary resin com-
interactions, including: elution of residual monomers or other posites invites further study. These composites incorporate
leachable components [1], degradation of bonds in the poly- some varied structural features, including: a silorane-based
mer networks or at resin-filler interfaces [2], uptake of water matrix, a high molecular mass and long matrix monomer
molecules into materials [3]. Such water sorption has been DX-511 and a self-adhering monomer. This paper investi-
established as a diffusion-controlled process [4–9]. During gates the exact functional relationship between hygroscopic
this process, ‘unbound’ water molecules diffuse into the expansion and water uptake over 150 d for each of these com-
matrix and, at the meso-scale, progressively occupy free vol- posites, via Type A plots, during water sorption/desorption
ume. During that initial phase, hygroscopic expansion and cycles.
plasticization may occur to a lesser extent than at later The null hypothesis was that: the functional dependence of
stages when free volume has been fully occupied. How- hygroscopic expansion on water uptake was completely linear
ever, ‘bound’ water molecules, produced by their interaction over the full range of water uptake for all materials investi-
with polymer chains through hydrogen bonds, can disrupt gated.
inter-chain hydrogen bonding, and facilitate absorption of
more water molecules. This may cause hygroscopic expansion
and plasticization and these time-dependent effects might
weaken mechanical properties [10,11] and thus increase wear 2. Materials and methods
rate [12,13].
On the other hand, a potentially beneficial effect of Five commercial materials were chosen to represent a range
hygroscopic expansion is that it might compensate for of restorative resin composites (Table 1).
polymerization shrinkage [14–16]. However, some marginal
adaption measurements indicate that polymerization shrink-
age cannot always be compensated by hygroscopic expansion
2.1. Specimen preparation
[17]. Conversely, there seems to be stronger recent evidence
that in less hydrophobic restoratives hygroscopic expansion
Twenty-five (n = 5) disk-shaped specimens, (15.0 ± 0.1) mm in
can be greater than the shrinkage and thus cause expansion
diameter by (2.0 ± 0.1) mm in thickness, were prepared accord-
stress, which may induce micro-cracks or even cracked cusps
ing to International Standard ISO FDIS 4049: 1999 [21] and the
in the restored tooth [15,18].
manufacturer’s instructions. In a laboratory environment at 23
There are, in principle, two possible types (A and B) of plot,
(±1) ◦ C and relative humidity of 50 (±2)%, uncured materials
which are nevertheless quite different, relating hygroscopic
were carefully dispensed into a brass ring mold and clamped
expansion and water uptake (Fig. 2a and b). Type A – pro-
between two glass slides covered by two pieces of polyester
duced for each individual composite – presents a ‘correlation
film. Then the apparatus were exposed to a halogen curing
over time’ between its expansion and water uptake (Fig. 2a),
light with 11 mm exit window (Optilux 501, Kerr Corporation,
whilst Type B involves data for a set of composites and corre-
USA), using a standard curing mode (output wavelength range:
lates the ‘maximum measured’ expansion and water uptake
400–505 nm; output irradiance: 580–700 mW/cm2 ). Specimens
for each member of the set (Fig. 2b). Linear regressions of
were carefully removed and any with visual defects were
Type A, between the dimensional change and amount of water
excluded. Any excess material was removed by grinding with
sorption, for six self-curing restorative resin composites were
1000 grit silicon carbide abrasive paper until visually smooth.
reported by Hirasawa et al. [19]. However, they only presented
The specimens were stored in a lightproof desiccator at
7 d data, which now would be an insufficient measurement
(37 ± 1) ◦ C for 22 h, and then transferred to another desic-
period for some contemporary resin composites. A linear
cator at (23 ± 1) ◦ C for 2 h. Each specimen was weighed by
dependence with Type B plots (first cycle: R2 = 0.98, second
a calibrated analytical balance with a precision of 0.01 mg.
cycle: R2 = 0.998) between percentage absorbed water and vol-
The completion of polymerization and dehydration was
umetric increase was reported for light-cured dimethacrylate
reached when the mass change of each specimen was within
resins [20]. Another study showed that hygroscopic expan-
0.1 mg in a 24 h period. This recorded constant mass (m1 )
sion was strongly correlated with water sorption (R2 = 0.98)
was the initial mass. Perspex control specimen disks were
in two compomers, one giomer and one resin composite [3].
used (Polymethylmethacrylate, Imperial Chemical Industries,
However, essentially no correlation (Pearson correlation coef-
UK).
ficient = 0.1675) was found between maximum water sorption
e220 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226

O O

O Si
Si O OH
O Si
Si
O P OH
O

O O

O O
O O

Silorane GPDM

O O

O NH O
O NH O
O O

UDMA
O

O C NH
O O
O
NH C O
O
O m'
NH C O O

O O n O

O C NH
O m

O DX-511
Fig. 1 – Chemical structures of the main organic matrices.

2.2. Water sorption/desorption m3 (t) − m1

Md (%) = × 100 (2)
m1
The specimens were randomly placed in 10 mL de-ionized
water at (37 ± 1) ◦ C in individual glass vials and were weighed 2.3. Hygroscopic dimensional changes
as a function of different immersion intervals until equilib-
rium was reached by 150 d. At different time points, each In parallel with the measurement of water sorption, the hygro-
specimen was carefully dried by filter paper, weighed to scopic expansion of the same specimens was monitored by a
±0.01 mg, and returned to fresh water storage. The recorded laser scan micrometer (LSM) described previously [22]. This
mass was noted m2 (t). Then the specimen was reconditioned measures the size of each disk specimen rapidly (<30 s) over
in the above desiccators over a 40 d period until constant mass multiple diameters to a resolution of 200 nm. The diametral
was obtained. Similarly, the recorded mass at different desorp- value presented for each disk at each time point was an overall
tion time points was noted m3 (t). The percentage apparent average of 445 data values. The grand mean dimension of the
mass change during water sorption – Ms (%) and desorption five disks per group was obtained at each sorption time point.
– Md (%) was calculated by: The initial diameter of each specimen was measured and
noted d1 . The diameter measured at time t during water
m2 (t) − m1 sorption was recorded as d2 (t) and the corresponding diam-
Ms (%) = × 100 (1)
m1 eter during water desorption was noted d3 (t). The percentage
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226 e221

Table 1 – Test materials.

Code Material Manufacturer Lot no./shade Filler loading Fillers Organic matrix
(Wt %)
FS Filtek® 3M ESPE, St. Paul, 20080514 76 Quarz (silane layer), Silorane
Silorane MN, USA A3 Radiopaque Yttrium
fluoride
GDA GC Gradia® GC Dental 0901134 73 Silica, Prepolymerized UDMA and
Direct Products Corp., A3 filler dimethacrylate
Anterior Tokyo, Japan co-monomers
GDP GC Gradia® GC Dental 0905201 77 Silica, Prepolymerized UDMA and
Direct Products Corp., A3 filler, dimethacrylate
Posterior Tokyo, Japan Fluoro-alumino-silicate co-monomers
glass
GCK GC Kalore GC America Inc., 0903171 82 Prepolymerized filler DX-511, UDMA and
USA A3 (with Lanthanoid dimethacrylate
Fluoride), co-monomers
Fluoro-alumino-silicate
glass, Strontium/Barium
glass, Silicon dioxide,
Lanthanoid fluoride
VF Vertise® Flow Kerr Corporation, 3172311 70 Prepolymerized filler, GPDM, HEMA and
Orange, CA, USA A2 Barium glass, methacrylate
Nano-sized colloidal co-monomers
silica, Nano-sized
Ytterbium fluoride
Silorane, 3,4-Epoxycyclohexylethylcyclo-polymethylsiloxane, bis-3,4-epoxycyclohexylethyl-phenylmethylsilane; UDMA, 1,6-
bis(methacrylyloxy-2-ethoxycarbonylamino)-2,4,4-trimethylhexane/Urethane Dimethacrylate; GPDM, glycerol phosphate dimethacrylate.

diametral change of water sorption – ds (%) and desorption – The time-dependence of mass-change and volumetric
dd (%) were given by: change during the water sorption/desorption cycles, for each
composite, are shown in Fig. 3a–e.
d2 (t) − d1 The relationships, for each material, between hygroscopic
ds (%) = × 100 (3)
d1 dimensional expansions and mass changes during water
sorption are shown as Type A plots in Fig. 4a–e. To a first
d3 (t) − d1
dd (%) = × 100 (4) approximation, these plots can be considered as being ‘near-
d1
linear’ and high Pearson correlation coefficients are presented
Thus the percentage hygroscopic dimensional change (volu- in Table 3. However, on closer inspection, some non-linearity
metric change) can be calculated by the following equation, is apparent in the initial phase of water uptake. That is,
assuming isotropic expansion in three dimensions. the initial expansion ‘rate’ was lower with respect to mass
uptake.
 3 
d(%)
V(%) = 100 1+ −1 (5)
100

2.4. Statistical analysis

The percentage mass change and volumetric change were cal- Table 2 – Percentage mass change and hygroscopic
culated for each group. Repeated measures ANOVA was used expansion (standard deviation) of test materials after
150 d immersion in de-ionized water at 37 ◦ C (p < 0.05).
for mass change and volumetric change (p < 0.05), one-way
ANOVA was performed for the percentage mass change and Material % mass change % hygroscopic
hygroscopic expansion at 150 d (p < 0.05), succeeded by Tukey’s expansion
a e
post hoc test. Pearson correlation coefficients were calculated Filtek® Silorane 0.68 (0.02) 0.74 (0.05)
b f
to analyze the correlation between hygroscopic expansion and GC Gradia Direct Anterior 1.92 (0.04) 1.90 (0.05)
c g
GC Gradia Direct Posterior 1.33 (0.02) 1.51 (0.07)
mass change for each test material during 150 d water immer- c f
GC Kalore 1.40 (0.09) 2.03 (0.07)
sion (two-tailed, p < 0.01). * d ** h
Vertise® Flow 2.83 (0.11) 4.79 (0.18)
Difference between groups having the same superscript letter was
3. Results not significant.
∗
The highest mass change [2.91% (±0.07)] of VF was reached at 42
The maximum mass changes and expansions of the com- d water immersion.
∗∗
The highest hygroscopic dimensional expansion [4.82% (±0.13)]
posites are presented in Table 2. Statistically significant
of VF was reached at 90 d water immersion.
differences between materials were as noted in this table.
e222 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226

a 2.0 terms of the well known theory that water molecules absorb
into microvoids and free volume within the resin matrix, with-
out creating significant expansion [2]. However, another factor
producing low early values of ∂v/∂m might be eluted compo-
% volumetric expansion

1.5
nents [24], the space of which could be re-occupied by water
molecules [18].
1.0 However, during the later stage, from 3 d to 150 d, and
especially in the case of FS, GDA and GDP (Fig. 4a–c), the
regression line increased almost linearly, suggesting a directly
.5 proportional effect of water sorption on hygroscopic expan-
sion, (Table 3). This trend was not as strong for GCK and VF,
for which the overall curves were slightly sigmoidal. Thus the
0.0 null hypothesis was rejected.
0.0 .5 1.0 1.5 2.0 The primary factor affecting the water sorption process
is the polymer system of each resin composite [2,25]. Water
% mass change
diffusion in polymer networks depends not only on the
molecular-sized holes in the network structure but also on
b 5 the affinity between the polymer and water molecules, which
are related to the degree of conversion and the presence
of hydrophilic groups respectively [9,26]. Other factors that
% volumetric expansion

4
influence the water sorption and hygroscopic expansion pro-
cess include: the type, size, morphology and fraction of the
3 filler; as well as the properties of the resin-filler interface, the
catalyst and initiator systems, the exposed surface area to
2 water and any bulk constraint (force) exerted on the materials
[2,5,6,27–32].
FS had the lowest mass change and hygroscopic dimen-
1
sional change during the water sorption/desorption cycle
(Fig. 3a). The major reason was that FS incorporated a silo-
0 rane monomer combined from hydrophobic siloxane and
0 1 2 3 4 5
low shrinkage ring-opening oxirane [33]. Extensive cross-
% mass change linking and rigid polymer chains, which can be expected to
increase the elastic modulus, may limit chain movements [34].
Fig. 2 – (a) Correlation over time for one composite. (b) A set Therefore the high cross-linking density generated from the
of composites: correlating their maximum measured photo-activated cationic polymerization in FS could probably
expansion and water uptake. hinder water diffusion and hygroscopic expansion. Mean-
while, the internal stress might be partially relieved and a
long-term stability of resin-filler interfaces could be expected
4. Discussion [28,33,35]. The findings of the current study concur with others
that a silorane-based composite presented amore hydropho-
This study found specific relationships between hygroscopic bic behavior than methacrylate-based composites [8,41].
expansion and mass change, which provided curves with gen- The water sorption and hygroscopic expansion of materials
erally similar shapes during 150 d water sorption (Fig. 4). The with the same resin matrix may depend on the filler con-
findings are consistent with previous studies [18–20,23]. How- tent, the nature of filler particles, the coupling agents and the
ever, the relationship was not exactly linear, particularly at incompletely covered sites on filler surface [36–38]. In terms of
the early stage. At this early period we explain the behavior in GDA and GDP (Table 1), more filler loading means less polymer
content. Because a more hydrophobic silane treatment, rather
than conventional silanol treatment, was applied to the silica
surfaces in GDA and GDP, the main difference between them
Table 3 – Pearson correlation coefficients between was probably the polymer content, causing the mass uptake
hygroscopic expansions and mass changes of test
and hygroscopic expansion of GDA to be slightly higher than
materials during 150 d immersion in de-ionized water at
37o C (p < 0.01). that for GDP.
VF had the greatest water sorption and hygroscopic expan-
Material Pearson p value
sion after 150 d. The secondary hydrogen bonds formed
correlation (2-tailed)
coefficient between the polar hydroxyl, carboxylate or phosphate groups
of polymer and water molecules will break previous inter-
Filtek® Silorane 0.978 0.000
chain hydrogen bonds and increase the mobility of chain
GC Gradia Direct Anterior 0.990 0.000
GC Gradia Direct Posterior 0.988 0.000
segments in polymer [39]. With the hydrophilic monomers
GC Kalore 0.992 0.000 GPDM and HEMA, more inter-chain hydrogen bonds were
Vertise® Flow 0.994 0.000 available for disruption in VF than for the other materials. In
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226 e223

(a) (b)
1.0 1.0 2.0 2.0

0.8 0.8 1.5 1.5

% volumetric change
% volumetric change

% mass change
% mass change

0.6 0.6
1.0 1.0

0.4 0.4
0.5 0.5

0.2 0.2
0.0 0.0
0.0 0.0
0 50 100 150 200 0 50 100 150 200
time(d) time(d)

(c) (d)
1.6 1.6
2.0 2.0
1.4 1.4
1.2 1.2
% volumetric change

% volumetric change
1.5 1.5
% mass change

1.0 1.0 % mass change

0.8 0.8
1.0 1.0
0.6 0.6
0.4 0.4
0.5 0.5
0.2 0.2
0.0 0.0
0.0 0.0
0 50 100 150 200 0 50 100 150 200
time(d) time(d)

(e)
5 5

4 4
% volumetric change

3 3
% mass change

2 2

1 1

0 0

-1 -1
0 50 100 150 200
time(d)

Fig. 3 – Percentage mass changes (filled circle) and volumetric changes (empty circle) of test materials during the water
sorption/desorption cycle. (a) Filtek® Silorane; (b) GC Gradia Direct Anterior; (c) GC Gradia Direct Posterior; (d) GC Kalore; (e)
Vertise® Flow.

addition, a statistically significant reduction in mass change suggest that the continuous solubility of VF [24] did not
was presented in VF after the peak value was reached at affect the hygroscopic expansion very much because of re-
42 d water immersion. However, no significant changes in occupation by water molecules, and so the volume of VF disk
hygroscopic expansion were shown after the maximum value could change along with water sorption concurrently but not
was attained at 90 d water immersion. The phenomenon simultaneously.
e224 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226

(a) 1.0 (b) 2.0

% volumetric expansion
0.8
% volumetric expansion

1.5

0.6
1.0
0.4

0.5
0.2

0.0 0.0
0.0 0.2 0.4 0.6 0.8 1.0 0.0 0.5 1.0 1.5 2.0
% mass change % mass change

(c) 1.6 (d)

1.4 2.0
% volumetric expansion

1.2

% volumetric expansion
1.5
1.0
0.8
1.0
0.6
0.4 0.5
0.2
0.0 0.0
0.0 0.2 0.4 0.6 0.8 1.0 1.2 1.4 1.6 0.0 0.5 1.0 1.5 2.0
% mass change % mass change

(e) 5

4
% volumetric expansion

0
0 1 2 3 4 5
% mass change

Fig. 4 – Relationships between volumetric expansion and percentage mass changes during 150 d water sorption of test
materials. (a) Filtek® Silorane; (b) GC Gradia Direct Anterior; (c) GC Gradia Direct Posterior; (d) GC Kalore; (e) Vertise® Flow.

The unusual disproportionate increase between volumet- linkages, and ester groups in polymers are hydrophilic
ric changes and mass changes of GCK and VF may be mainly because of their formation of hydrogen bonds with water
related to the incorporated monomers (Fig. 4d and e). The DX- [2]. The strength order of these hydrogen bonds depends
511 monomer in GCK has two flexible side arms (Fig. 1). The on the cohesive energy density of the polar groups
more flexible the polymer chains are, the greater the possi- (hydroxyl > urethane > ether) [40]. One DX-511 monomer
ble hygroscopic expansion of resin composites [40]. On the molecule in GCK has more urethane group (–NHCOO–) than
other hand, polar groups such as hydroxyl, urethane, ether one UDMA molecule in GDP (Fig. 1), which means the former
 d e n t a l m a t e r i a l s 2 9 ( 2 0 1 3 ) e218–e226 e225

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