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Selection of a composite resin based on high filler content, may be misleading. The reported
filler content may vary, depending on the ratio of prepolymerized resin to inorganic glass
particles. A composite material should be labeled with two values: total filler and inorganic
filler contents.
ensure dissolution of the organic matrix. The be used to identify the presence of that element
calculation of filler percentage by weight was the within the sample. The relative intensities of the
same as the ashing technique except that residual spectral peaks may be used to determine the relative
material might include prepolymerized fillers, clus- concentrations of each element in the specimen. The
ters, and possible silane contents. The formula to x-ray signal is detected by a solid-state silicon-
determine percentage by weight of the specimens lithium detector, and the construction and efficiency
after acetone dissolution was as follows: of this detector sets a lower limit on the atomic
number that may be detected. Generally, elements
Weight Wt percent heavier than carbon are detectable.22
Wt after dissolution Wt of tube For the SEM evaluation, the residual fillers from
3 100:
Initial Wt of sample ashing in air were mixed with acetone to produce a
suspension that was placed on an aluminum SEM
For the ashing in air, the filler content of the stub and allowed to dry. Morphologic and size
selected composites was determined by using a burn evaluations were done using a FEI Quanta 200 3D
out furnace (Neymatic 101, JM Ney Company, focused ion beam workstation and environmental
Bloomfield, CT, USA). Crucibles were weighed scanning electron microscope with an EDS system at
empty and then weighed after specimen loading magnifications of 20,0003 and 40,0003 at 20-30 kV
using an analytical scale (Analytical Standard, beam acceleration voltage. The same areas of the
AS200-S, OHaus, Florham Park, NJ, USA). The samples utilized for SEM observation were addition-
crucibles (High alumina, 10 mL, Cole-Palmer In- ally x-ray scanned using the same microscope for
strument Co, Golden, CO, USA) loaded with speci- qualitative and semi-quantitative analyses to deter-
mens were introduced in the furnace after the mine the elemental distribution profile.
temperature had reached 6508C and left for 30
minutes. The crucibles with the ashed specimens RESULTS
were again weighed on an analytical scale.
Table 2 shows the means and standard deviations of
Filler percentages from ashing in air and acetone the materials evaluated by ashing in air and acetone
dissolution technique were statistically analyzed by dissolution techniques. Weight percentage of inor-
one-way analysis of variance (ANOVA), independent ganic fillers from ashed specimens ranged from
t-tests, Tukey multiple comparison, and Pearson 70.62% to 86.44%. Weight percentage of fillers from
correlation. acetone dilution specimens ranged between 75.56%
EDS is a microanalytic technique that is based on and 85.05%. Mean values for each material were
the characteristic x-ray peaks that are generated significantly different when comparing ashing with
when the high-energy beam of the electron micro- acetone dissolution techniques. Both techniques
scope interacts with the specimen. Each element were extremely precise, with standard deviations
yields a characteristic spectral fingerprint that may between 0.1% and 1.1%. Aelite LS and Filtek LS
Figure 1. (A): SEM photomicrographs and filler measurements of IPS Empress Direct composite after acetone dissolution at 40,0003 magnification.
(B): SEM photomicrographs and filler measurements of Filtek LS composite after acetone dissolution at 40,0003 magnification. (C): SEM
photomicrographs and filler measurements of Kalore composite after acetone dissolution at 40,0003 magnification. (D): SEM photomicrographs and
filler measurements of Aelite LS composite after acetone dissolution at 40,0003 magnification.
showed closer results for percentages by weight to ashing in air and acetone dilution. Both techniques
manufacturers reported data when using ashing were highly correlated (r=0.72).
(2%) and acetone technique (1%-3%). On the other Representative SEM photomicrographs (backscat-
hand, Kalore and IPS Empress Direct showed tered electron images) of the composites evaluated in
this study at 40,0003 are shown in Figure 1A
results closer to manufacturer reported data when
through D. Irregular particles (3.96 lm) in conjunc-
using acetone dilution for weight measurements tion with smaller spherical (32.03 nm-2.22 lm) filler
(0%-5%). Aelite LS had a significantly higher loading particles and agglomerated particles were observed
than the others for weight percentage for both in Aelite LS. Overall, Aelite LS was the material that
Salazar, Dennison & Yaman: Filler Analysis of Four Resin Composites E205
Figure 2 (A): SEM photomicrographs used for EDS analysis and color mapping obtained by the superimposition of every individual element
distribution in the IPS Empress Direct composite: Si-yellow, Al-pink, O-purple, F-green, Yb-red, Ba-light blue. (B): SEM photomicrographs used for
EDS analysis and color mapping obtained by the superimposition of every individual element distribution in the Filtek LS composite: Si-pink, Mg-blue,
Al-purple, F-green, O-red, Y-light blue. (C): SEM photomicrographs used for EDS analysis and color mapping obtained by the superimposition of
every individual element distribution in the Kalore composite: Si-pink, Al-purple, Mg-blue, F-green, O-yellow, Yb-light blue. (D): SEM
photomicrographs used for EDS analysis and color mapping obtained by the superimposition of every individual element distribution in the Aelite
LS composite: Si-blue, Al-red, O-light blue.
showed the biggest (3.96 lm) and smallest filler observed, with particles typically ranging from 1.28
particles (32.03 nm) (Figure 1D). Irregular and lm to 1.77 lm, and the smallest particles being
splintered filler particles of different sizes were seen around 56.62 nm (Figure 1A). The elements detected
in Filtek LS, IPS Empress Direct, and Kalore. In in the resin composites are shown in Figure 2A
Filtek LS, most of these particles were somewhat through D and Table 3. Silica, aluminum, and
larger (598 nm-2.74 lm), while the remaining oxygen were found in all of the resin composites
particles were between 212.77 nm and 321.61 nm tested and were the main components of the fillers.
(Figure 1B). Kalore showed the most regularly
shaped filler particles among all composites evalu- DISCUSSION
ated, with a mix of medium (631 nm-1.85 lm) and
small (48 nm-157 nm) size particles (Figure 1C). On Many methods could be used to study the filler
the other hand, in IPS Empress Direct, a more concentration by weight. Thermogravimetry is a
irregular shape pattern in the filler particles was technique in which the mass of a material is
E206 Operative Dentistry
percentages of fillers.8 Some manufacturers seem to For Filtek LS, the SEM images confirmed a
evaluate the percentage of fillers by weight before distinct filler morphology of irregularly shaped
the silanization process of the fillers, while others fillers. The manufacturer of Filtek LS claimed that
include the percentage of silane coating in their the radical change in the shape of the fillers, among
calculation. In addition, the surface area of the fillers the Filtek composite varieties, is related to the
will affect the percentage of silane usedthe smaller specific characteristic that the silorane-based organ-
the fillers, the higher the quantity of silane. ic matrix needs in its composition. Silorane is known
to contain quartz particles, which cannot be pro-
Furthermore, samples from each composite were
cessed by a sol-gel technique and may explain the
dissolved in acetone to evaluate the filler content by
more irregular morphology compared with other
weight using a technique that preserves the prepo-
materials provided by the same manufacturer.
lymerized particles. Previous studies had evaluated According to the manufacturer, the average size
filler structure and size,8,10,11,22,24 but only one range was from 40 nm to 1700 nm; however, the
previous study has determined filler percentage by SEM images in this study showed particles that
weight using the acetone dissolution technique.17 ranged from 200 nm to 3 lm in size. In addition, the
With the new generation of composites, it will be images showed a more heterogeneous size pattern
necessary to evaluate these materials considering when compared to Kalore, the other microhybrid
their prepolymerized particles. A pilot study was material.
done to determine the amount of cycles of acetone
According to the manufacturer, Kalore contains
dissolution necessary to obtain a stable percentage
60% filler content by weight of 400 nm nano-sized
by weight. No significant differences were found
modified strontium glass and 20% filler content by
between the second and third dissolution; therefore,
weight of 100 nm of lanthanoid fluoride. Prepoly-
two cycles of acetone dissolution were chosen as a
merized nanoclusters of fillers, inorganic fillers, and
standard procedure. Kalore showed the highest
mono-dispersed particles, contained in this specific
difference in filler content by weight for the acetone nanohybrid composite present size ranges between
dissolution technique (77.73%). A similar increase 16 nm and 17 lm. When the samples were evaluated
was seen with IPS Empress Direct when comparing under SEM, the images showed more regular shaped
ashing in air (72.17%) and acetone dissolution filler particles whose bigger particles ranged from
(78.88%). Aelite LS and Filtek LS showed a 632 nm to 1.8 lm and small particles ranged from 48
decreased weight percentage when using acetone nm to 158 nm. Among all materials, Aelite LS (32
dissolution, which may be related to residual nm) and Kalore (48 nm) are the materials that had
nanoparticles suspended in the acetone after centri- the smallest filler particles in their structure. In
fuge sedimentation that are lost during pipette addition to Kalore and Fitek LS, IPS Empress Direct
aspiration. also showed irregular shaped particles with large
For the filler morphology analysis, the samples fillers that ranged from 1.28 lm to 1.77 lm and
dissolved in acetone were collected and dissolved a smaller aggregates of particles with sizes from 56.62
third time for mounting purposes. On the SEM nm to 196.97 nm.
evaluation, all composites showed an irregular to In this study, prepolymerized particles were not
splintered shape except for Aelite LS, which is the evaluated for elemental analysis because the com-
only composite in this study that contains spherical ponents of each composite material were disrupted
particles mixed with irregular-shaped particles. A during the acetone dissolution technique; therefore,
spherical shape is known to have many advantages further studies should be done keeping the organic
such as to allow an increased filler load for matrix of each resin-based composite.
composites and also to enhance their fracture Many modifications have been made recently to
strength, surface roughness, and shrinkage strain the elemental composition of filler particles. Ele-
since mechanical stresses tend to concentrate on the ments such as aluminum and lithium were added to
angles and protuberances of the filler parti- decrease the hardness on these particles, to be able
cles.3,8,10,31,32 The spherical particles had different to break them in smaller sizes. Barium, yttrium,
diameters that ranged from 32 nm to 2 lm, while the zinc, and strontium are added to develop radiopacity.
bigger irregularly shaped particles presented an Some manufacturers have claimed that yttrium
average size of 4 lm with some nanoclusters and fluoride can be incorporated to release fluoride ions
dispersed nanoparticles surrounding the bigger filler for anticaries activity.21 In this study, the EDS
particles. analysis of the fillers revealed a variety of elements,
E208 Operative Dentistry
depending upon the individual products. Colors 2. Aelite LS had significantly higher filler content for
representing each element were picked randomly both ashing and acetone dissolution.
for each analysis (Table 3, Figure 2). 3. Kalore had significantly lower filler content for
For IPS Empress Direct (Figures 1A and 2A), the ashing (70.62%), and Filtek LS had significantly
filler particle sizes are well dispersed, and the lower filler content for acetone dissolution
predominant elements of silica (yellow) and fluoride (75.56%).
(green) appear to be concentrated in the larger 4. Manufacturer reported filler content for Aelite LS
particles; ytterbium (red) and barium (light blue), (88%) and Filtek LS (76%) approximated the study
however, appear to be in smaller, more dispersed results for both techniques, while Kalore (82%)
particles. Aluminum is generalized throughout the and IPS Empress Direct (79%) were only similar
field, in keeping with the stud background on which for acetone dissolution, indicating higher content
the fillers were placed. of prepolymerized particles.
5. Morphologic examination showed spherical
For Filtek LS (Figures 1B and 2B), the particles
shaped particles for Aelite LS and splintered
are larger and more distinct (Figure 1B). Silica
and irregular shaped particles for the other
(pink) and oxygen (red) are heavily concentrated in
materials.
the more distinct larger particles (Figure 2B), and
6. The elements detected were silica (Si), aluminum
separate less numerous particles contain a high
(Al), strontium (Sr), yttrium (Y), magnesium (Mg),
concentration of fluoride (green) as well as magne-
fluorine (F), ytterbium (Yb), oxygen (O), zirconium
sium (blue) and yttrium (light blue) for radiopacity.
(Zr), and barium (Ba). Si, Al, and O were the
Again, the aluminum (purple) forms the general
common elements in the composition of all four
background color from the mounting stub.
resin composites evaluated.
For Kalore (Figures 1C and 2C), the larger 7. Manufacturers should provide two filler content
particles appear to contain heavier concentrations values for a composite resin materialinorganic
of ytterbium (light blue) and magnesium (blue) with filler content and total filler content.
some aluminum (purple) microconcentrations within
specific particles. Other particles appear to contain
Conflict of Interest
heavier concentrations of silica (pink). Small
amounts of fluoride (green) were distributed around The authors of this manuscript certify that they have no
proprietary, financial, or other personal interest of any nature
the edges of most particles, and there was no oxygen or kind in any product, service, and/or company that is
(yellow) evident in most fields. presented in this article.
For Aelite LS (Figures 1D and 2D), the predom-
(Accepted 12 February 2013)
inant element is silica (blue) in both larger and
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