Construction and Building Materials 43 (2013) 242–252

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Construction and Building Materials

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Evaluation of natural zeolite as warm mix asphalt additive and its comparison
with other warm mix additives
Burak Sengoz a,⇑, Ali Topal a, Cagri Gorkem b
a
Dokuz Eylul University, Department of Civil Engineering, Faculty of Engineering, 35160 Buca, Izmir, Turkey
b
Dokuz Eylul University, Graduate School of Natural and Applied Sciences, 35160 Buca, Izmir, Turkey

h i g h l i g h t s g r a p h i c a l a b s t r a c t

" The addition natural and synthetic

zeolites reduce mixing and
compaction temperature.
" Natural zeolite can be used as an
alternative WMA additive to
synthetic zeolite.
" WMA additives increase the elastic
characteristics of the bitumen.
" 5% zeolites, 3% organic and 2%
chemical additive are considered as
optimum contents.

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

Article history: In last decade, warm mix asphalt (WMA) has been used as alternative to hot mix asphalt (HMA) that
Received 22 January 2013 reduces the temperature of asphalt during production and placement, minimizes greenhouse gases while
Received in revised form 13 February 2013 maintaining the advantages of HMA. This study targets the investigation of natural zeolite as a WMA
Accepted 20 February 2013
additive and its comparison with different types of WMA additives (organic, chemical and synthetic zeo-
Available online 22 March 2013
lite). The bitumen samples have been produced by mixing a 50/70 penetration grade bitumen with dif-
ferent types of WMA additives at various contents. The fundamental and rheological properties of
Keywords:
bitumen samples involving different types of WMA additives have been determined by using conven-
Warm mix asphalt
Natural zeolite
tional bitumen test methods and dynamic shear rheometer (DSR).
Synthetic zeolite Ó 2013 Elsevier Ltd. All rights reserved.
Organic additive
Chemical additive

1. Introduction ergy consumption due to the reduction of mixing and compaction

In recent years, environmental consciousness is becoming a sig-
nificant issue in asphalt production with the increase in demand of
new highway networks. Although hot mix asphalt (HMA) is widely
used in whole over the world, some recent investigations suggest
using another process that reduces the amount of greenhouse
gases emissions by reducing the fuel used during production (en-
⇑ Corresponding author. Tel.: +90 232 301 7072; fax: +90 232 301 7253.
E-mail address: burak.sengoz@deu.edu.tr (B. Sengoz).
temperatures), improves workability and obtains a strength and
durability that is equivalent to or better than HMA [1–3]. Based
on this idea, a number of new processes and products have been
developed. One of these technologies is called warm mix asphalt
(WMA). WMA is a type of asphalt which is mixed at temperatures
lower than conventional asphalt. Typically, the mixing tempera-
tures of WMA range from 100 to 140 °C (212–280 °F) compared
to the mixing temperatures of 150–180 °C (300–350 °F) for a con-
ventional asphalt [4,5].

0950-0618/$ - see front matter Ó 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.conbuildmat.2013.02.026
 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252 243

Table 1
The properties of the base bitumen.

Test Specification Results Specification limits

Penetration (25 °C; 0.1 mm) ASTM D5 63 50–70
EN 1426
Softening Point (°C) ASTM D36 49 46–54
EN 1427
Viscosity at (135 °C), Pa s ASTM D4402 0.51 –
Thin film oven test (TFOT); (163 °C; 5 h) ASTM D1754
EN 12607-1
Change of mass (%) 0.07 0.5 (max)
Retained penetration (%) ASTM D5 51 50 (min)
EN 1426
Softening point after TFOT (°C) ASTM D36 51 48 (min)
EN 1427
Ductility (25 °C; cm) ASTM D113 100 –
Specific gravity ASTM D70 1.030 –
Flash point (°C) ASTM D92 260+ 230 (min)
EN 22592

Table 2
Physical properties and chemical structure of natural zeolite.

SiO2 Al2O3 Fe2O3 K2O H2O CaO MgO Na2O Ti Ag N B (ppm)

Chemical structure
Content (%) 71.29 13.55 1.15 3.5 5.9 1.96 0.7 0.6 0.02 0.04 30

Physical properties
Voids (%) Dimensions of the main channels (A) Thermal stability Ion exchange capacity (meq/g)
34 3.9  5.4 High 2.16

Table 3
Conventional properties of bitumen prepared with warm mix asphalt additives.

WMA Contents Pen. Softening Viscosity Thin film oven test (TFOT) Rolling thin film oven test (RTFOT) Storage
types (%) (0.1 mm) point (°C) (mPa s) stability
(°C)
135 °C 160 °C Loss of Retained Soft. point Loss of Retained Soft. point Pen.
mass (%) pen. (%) diff. (°C) mass (%) pen. (%) diff. (°C) index
(PI)
Natural 0 55 49.1 412.5 137.5 0.04 25 5.0 0.04 26 5.3 1.20
zeolite
3 54 53.6 362.5 162.5 0.16 18 4.1 0.16 22 4.4 0.16 1.6
4 53 54.1 350.0 125.5 0.16 17 4.0 0.17 18 4.3 0.10 1.8
5 51 55.0 325.0 113.0 0.16 15 3.7 0.17 17 3.7 0.02 2.0
6 45 58.2 400.0 187.5 0.17 10 3.5 0.17 15 3.2 0.40 2.4
7 42 59.2 487.5 187.5 0.17 10 3.2 0.17 13 3.0 0.44 2.4
Synthetic 0 55 49.1 412.5 137.5 0.04 25 5.0 0.04 26 5.3 1.20
zeolite
3 55 53.1 350.0 138.0 0.15 18 4.9 0.16 23 5.0 0.26 1.4
4 53 53.6 325.0 125.0 0.15 17 4.7 0.17 21 4.8 0.22 1.6
5 52 56.0 312.5 112.5 0.16 16 4.1 0.18 21 4.5 0.27 1.6
6 45 59.9 437.5 150.0 0.16 11 3.3 0.18 14 3.7 0.74 2.2
7 43 61.2 512.5 175.0 0.17 10 3.2 0.18 13 3.2 0.87 2.4
Organic 0 55 49.1 412.5 137.5 0.04 25 5.0 0.04 26 5.3 1.20
2 43 61.2 300.0 112.0 0.07 14 4.3 0.07 16 4.5 0.89 1.8
3 37 69.3 287.5 75.0 0.07 13 4.0 0.07 15 4.3 1.95 1.6
4 31 79.5 275.0 75.0 0.08 6 2.5 0.08 10 3.5 3.07 1.6
Chemical 0 55 49.1 412.5 137.5 0.04 25 5.0 0.04 26 5.3 1.20
1 48 55.4 350.0 113.0 0.06 19 3.4 0.06 22 3.6 0.04 2.2
2 44 56.7 337.5 87.5 0.04 16 2.5 0.07 17 2.5 0.04 0.5
3 40 58.0 287.5 75.0 0.06 13 1.5 0.08 17 2.1 0.09 0.6

The initial studies in the field of WMA have begun as foaming of
the bitumen by Csanyi in 1956 [6]. This study was one of the first
successfully steam injection into bitumen to create a foaming
mass. Based on the method, the bitumen is introduced into a mixer
in atomized form and aggregate is passed through the cloud of
atomized bitumen. It was a natural progression that led to the
development of a system where the bitumen is foamed before it
contacts with mineral aggregate.
The modern investigations about WMA start with German Bitu-
men Forum in 1997 [7]. The aim of the forum was to become famil-
iar with WMA technology for the bitumen manufacturers by the
help of limited investigated studies. Following the forum, in accor-
dance with the requirements of manufacturers, the researchers
have begun detailed investigations which involve the addition of
organic additives, chemical additives and foaming with water in
mineral [3].
244 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252

Table 4
Mixing and compaction temperatures of WMA additives.

Additives Contents Mixing temp. Compaction temp.

(%) (°C) (°C)
Base bitumen (AC 0 156–163 143–149
50/70)
Natural zeolite 3 158–168 141–149
4 153–160 139–142
5 150–157 137–142
6 165–174 145–154
7 164–172 149–156
Synthetic zeolite 3 155–162 139–146
4 152–159 136–143
5 149–152 135–142
6 158–165 145–151
7 163–169 149–155
Organic 2 149–156 134–140
3 144–149 134–138
4 144–149 132–137
Chemical 1 151–157 138–144
2 148–153 173–142
3 144–150 133–138

WMA technology can be classified based on the utilization of
organic and chemical additives as well as on the utilization of
water. Organic additives are used to achieve temperature reduc-
tion by reducing the viscosity of bitumen. A decrease of viscosity
produces asphalts at low temperatures. After crystallization, the
stiffness of the bitumen increases making and asphalt’s resistance
better against deformation [3,8].
Chemical additives are combination of emulsification agents,
polymers and additives to enhance workability, compaction and
adhesion. The contents of chemical additive used in bitumen were
generally based on the recommendations by the suppliers as well
as literature [3,5].
Utilization of water for WMA can be classified into two major
groups; mainly the direct injection of water to the bitumen and
the utilization of hydro-thermally crystallized minerals such as
zeolites. Synthetic zeolite is a finely powdered hydrated sodium
aluminum silicate that is hydro-thermally crystallized, and it holds
18–22% (by mass) of water. Theoretically, the zeolite releases
water which creates foam that reduces the viscosity and increases
the workability. It facilitates better coatings of the bitumen on
aggregates.
Natural zeolites are microporous, hydrated aluminosilicate
minerals commonly used as commercial adsorbents [9,10]. Clinop-
tilolite is one of the most common natural zeolite comprising a
microporous arrangement of silica and alumina tetrahedra. It is
used in many applications such as a chemical sieve, gas absorber,
feed, food and fertilizer additive, a soil amendment as well as used
in the production of pozzolan cement and concrete in buildings.
Clinoptilolite is well conformed to these applications due to its
large amount of pore space, high resistance to extreme tempera-
tures and chemically neutral basic structure. Most of the clinoptil-
olite ore beds are located around the Aegean Sea Region [11]. In
addition, Turkey has the necessary environmental geological activ-
ity for the formation of natural zeolites and it is estimated that
there are nearly 50 billion tons of natural zeolite ore.
This study aims to characterize the properties of bitumen sam-
ples involving clinoptilolite type of natural zeolite and other types
of warm mix additives (synthetic zeolite, organic and chemical)
with their different contents. For this purpose conventional test
methods as well as dynamic shear rheometer (DSR) at different
temperatures and low and high frequency level have been
performed.

Fig. 1a. Complex modulus of natural zeolite at 0.01 Hz.

 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252 245

Fig. 1b. Complex modulus of natural zeolite at 10 Hz.

2. Experimental
2.1. Materials
The base bitumen with a 50/70 penetration grade has been obtained from Ali-
aga/Izmir Oil Terminal of the Turkish Petroleum Refinery Corporation. In order to
characterize the properties of the base bitumen, conventional test methods such
as: penetration test, softening point test, and ductility test, have been performed.
These tests have been conducted in conformity with the relevant test methods that
are presented in Table 1.
Natural zeolite which can be considered as an alternative to synthetic zeolite
WMA additive has been supplied from a Turkish local company in powder form.
It has the complex formula: (Na3K3)(Al6Si30O72)
27H2O. It forms as white to reddish
tabular monoclinic tectosilicate crystals with a Mohs hardness of 3.5–4.0 and a spe-
cific gravity of 2.1–2.2. The content of natural zeolite in this study has been chosen
as 3–7% by weight of bitumen so as to compare its fundamental characteristics with
synthetic zeolite. The properties of natural zeolite are presented in Table 2.
There are various types of water-containing additive in market. In this study,
the North American hydro-thermally crystallized powdered synthetic zeolite has
been used. It contains about 18–21% water of crystallization which has released
by increasing temperature above 85 °C. The expansion of water causes foaming of
bitumen. The manufacturer of this type of synthetic zeolite has reported that the
utilization rate of synthetic zeolite in base bitumen varies between 3–7% by weight
of bitumen [3,12].
The organic WMA additive, which has been supplied from a South African com-
pany, is a long-chain aliphatic polymethylene hydrocarbon produced from the
Fischer–Tropsch (FT) chemical process with a melting temperature of 120 °C. The
longer chains help keep the wax in solution, which reduces bitumen viscosity at
typical asphalt production and compaction temperatures. The organic WMA addi-
tive concentrations in the base bitumen were chosen as 2–4%. The utilization of
these contents is based on past researches [3,7,13].
Chemical WMA additive, which has been used in this study, is a combination of
cationic surfactants and organic additive based rheology modifier. The additive
chemically modifies the bitumen and obtains active adhesion force that improves
coating of aggregates with bitumen [3,5,13]. Researchers have indicated that the
chemical WMA additive should be used at dosage rates of 1–3% by weight of the
bitumen for better performance of mixture [4,14–16].
2.2. Test methods
2.2.1. Conventional bitumen tests
The base bitumen and bitumen prepared with WMA additives have been
subjected to the following conventional bitumen tests; penetration (ASTM D5-
06), ring and ball softening point (ASTM D36-95), thin film oven test (TFOT)
(ASTM D 1754-97), penetration and softening point after TFOT and storage sta-
bility test (EN 13399) [17–20]. In addition, the temperature susceptibility of
the bitumen samples has been calculated in terms of penetration index (PI) using
the results obtained from penetration and softening point tests. The storage sta-

Fig. 2a. Complex modulus of synthetic zeolite at 0.01 Hz.

246 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252

Fig. 2b. Complex modulus of synthetic zeolite at 10 Hz.

bility value was determined by the difference of softening point temperatures of
bitumen samples taken from the top and bottom of cylindrical mold (32 mm
diameter and 160 mm height) after they were stored vertically at 163 °C in an
oven for 72 h.
2.2.2. Determination of mixing and compaction temperature
The effect of viscosity on workability of bitumen is very important in selecting
proper mixing and compacting temperatures.
Brookfield viscometer has been employed to measure the viscosity of bitumen
samples according to ASTM D4402-06 [21]. Approximately 30 g of bitumen have
been heated in an oven so that it was sufficiently fluid to pour into the sample
chamber. The amounts of bitumen used varied with the different sizes of the spin-
dles. The sample chamber containing the bitumen sample has been then placed in
the thermo container. After desired temperature has been stabilized for about
15 min, the spindle has been lowered into the chamber to test the viscosity. The test
was performed at 135 °C and 165 °C. The temperatures corresponding to bitumen
viscosities 170 ± 20 mPa s and 280 ± 30 mPa s were chosen as mixing and compac-
tion temperatures respectively.
2.2.3. Determination of rheological properties of WMA additives at different
temperatures and frequencies
The DSR test was performed on WMA samples by using a Bohlin Gemini II DSR
rheometer. The test was performed under controlled stress loading conditions using
low (0.01 Hz) and high (10 Hz) frequency sweeps at temperature between 30 °C and
80 °C (for every 10 °C). The stress amplitude for all the tests was confined within the
linear visco-elastic response of the bitumen.
3. Results and discussions
3.1. Conventional test methods
The conventional properties of the bitumen prepared with
water containing additives (natural and synthetic zeolites), organic
and chemical are presented in Table 3 as a decrease in penetration
and increase in softening point.

Fig. 3a. Complex modulus of organic WMA additive at 0.01 Hz.

 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252 247

Fig. 3b. Complex modulus of organic WMA additive at 10 Hz.

The increase in softening point is favorable since bitumen with
higher softening point may be less susceptible to permanent defor-
mation (rutting) [22]. Natural, synthetic zeolites, organic and
chemical WMA additives (for all contents) reduce temperature sus-
ceptibility (as determined by the penetration index – PI) of the
bitumen. Lower values of PI indicate higher temperature suscepti-
bility. As seen in Table 3, all WMA samples exhibit less tempera-
ture susceptibility compared to base bitumen with increasing
WMA additive content. Natural zeolite involving bitumen sample
exhibits satisfactory temperature susceptibility characteristics in
terms of PI values as presented in Table 3. Besides among all the
additives, the bitumen involving organic additive exhibits the low-
est temperature susceptibility. Asphalt mixtures containing bitu-
men with higher PI are more resistant to low temperature
cracking as well as permanent deformation [22].
Softening point test results on bitumen samples prepared with
WMA additives taken from the top and bottom of the tube in the
storage stability test indicate that, both natural and synthetic zeo-
lite involving bitumen samples exhibit similar storage stability
characteristics as presented in Table 3. Besides, the bitumen
samples prepared with chemical additives are much more storage
stable compared to other WMA samples.
3.2. Determination of mixing and compaction temperature
The viscosity values of samples involving WMA additives are
also seen in Table 3. Related to bitumen samples involving natural
and synthetic zeolite, the viscosity values decrease with the in-
crease in zeolite content up to 5% and decrease there on as pre-
sented in Table 3. Therefore, based on the viscosity data, 5% can
be evaluated as optimum for both natural and synthetic zeolite
content. The results also show a consistent decrease in viscosity
by the increase in WMA content for organic and chemical WMA
additive. This indicates that, all organic and chemical WMA addi-
tives increase the workability and make relatively reductions for
mixing and compaction temperatures.
The temperature corresponding to compaction and mixing
range is summarized in Table 4.
It is evident that addition of natural zeolite, synthetic zeolite,
organic and chemical WMA additives reduced the mixing

Fig. 4a. Complex modulus of chemical WMA additive at 0.01 Hz.

248 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252

Fig. 4b. Complex modulus of chemical WMA additive at 10 Hz.

Fig. 5a. Modification indices of natural zeolite at 0.01 Hz.

Fig. 5b. Modification indices of natural zeolite at 10 Hz.

B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252 249

Fig. 6a. Modification indices of synthetic zeolite at 0.01 Hz.

Fig. 6b. Modification indices of synthetic zeolite at 10 Hz.

Fig. 7a. Modification indices of organic WMA additive at 0.01 Hz.

250 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252

Fig. 7b. Modification indices of organic WMA additive at 10 Hz.

temperature by 6 °C, 9 °C, 13 °C and 9 °C respectively. Besides, the
addition of mentioned additives reduce the compaction tempera-
tures by 6 °C, 7 °C, 10 °C and 6 °C respectively.
3.3. Results of rheological properties of WMA additives at different
temperatures and frequencies
The variation of complex modulus (G) of the base bitumen and
the bitumen samples involving natural, synthetic zeolite and or-
ganic as well as chemical WMA additives at low (0.01 Hz) and high
frequency level (10 Hz) and at six different temperatures are pre-
sented in Figs. 1–4 respectively.
As depicted in Figs. 1–4, as temperature decreases, complex
modulus increases. An increment in G indicates higher elastic part,
thus an improved elastic behavior. Besides, for all bitumen sam-
ples, G increases with increase in frequency. This is due to the rhe-
ologic behavior of the bitumen samples since bitumen under
shorter loading times (high frequency level) exhibit elastic
behavior.
As illustrated in Figs. 1a and 1b, significant variation is achieved
in G values at low frequency level above 5% natural zeolite addi-
tion especially at 30 °C and 40 °C temperature level. This may be
due to the filler effect of natural zeolite utilization above 5%. The
mention variation becomes less significant on reaching high fre-
quency levels.
As seen in Fig. 2, no significant variation is seen in G values
with synthetic zeolite addition in comparison with base bitumen.
However, 5–6% synthetic WMA addition exhibits slightly higher
G at high frequency level at low temperature compared to other
contents.
G values of the samples involving organic WMA additive are
greater than G of base bitumen for all temperatures and frequen-
cies as seen in Figs. 3a and 3b. Besides, at both low and high fre-
quency and at all temperature levels, G increases with increase
in additive content as presented in Fig. 1. The variation of incre-
ment is more pronounced above 3% organic additive content at
low frequency level and especially low temperatures.
As depicted in Figs. 4a and 4b at 30 °C temperature and at all
frequency levels, 2% chemical WMA content exhibits greatest G
value.
Along with the complex modulus values, the effect of WMA
additives were also evaluated by the modification index (MI)
determined by the ratio of G of additive involving bitumen sam-
ples to G of base bitumen. The calculated MI values at low and
high frequency level as well as at six different temperature levels
are presented in Figs. 5–8.
Based on Figs. 5a and 5b, at both low and high frequency level
and at all temperatures, 6% natural zeolite WMA additive exhibit
the highest MI values.
No significant variation in MI values is observed with increase
in temperature at high frequency level as illustrated in Fig. 5b.

Fig. 8a. Modification indices of chemical WMA additive at 0.01 Hz.

 B. Sengoz et al. / Construction and Building Materials 43 (2013) 242–252
Fig. 8b. Modification indices of chemical WMA additive at 10 Hz.
However, similar trend cannot be achieved at low frequency level
as presented in Fig. 5a. As illustrated in both Figs. 5a and 5b, at a
constant temperature level and additive content, MI values of nat-
ural zeolite decrease with increase in frequency.
As illustrated in Fig. 6a, at low frequency level and at tempera-
tures below 60 °C, no variation is seen in MI values with increase in
synthetic zeolite content. However, temperature effect on MI is
more pronounced at high temperatures (above 60 °C) especially
for the bitumen sample involving 5% synthetic zeolite WMA
additive.
As depicted in Fig. 6b, at high frequency level and at all temper-
atures 5% synthetic zeolite WMA additive exhibits slightly higher
MI values compared to other contents.
As depicted in Figs. 7a and 7b, among all temperatures MI val-
ues increase with increase in organic additive contents for both
low and high frequency level. The variation of increment is more
pronounced above 3% organic WMA additive. Besides, at both
low and high frequency levels, MI values increase with increase
in temperature as depicted in Fig. 7.
Related to chemical additive presented in Fig. 8a, at low fre-
quency level, MI values increase with increase in chemical additive
content among all temperature level. However, a generalized trend
cannot be achieved on reaching high frequency level as depicted in
Fig. 8b.
Based on both low and high frequency level, MI values increase
with increase in temperature above 60 °C as seen in Fig. 8. At tem-
peratures between 40 °C and 60 °C, MI values exhibit the lowest
values. Besides, as illustrated in Fig. 8a, 3% chemical WMA additive
exhibits the highest MI values at all temperatures and at low
frequency.
4. Conclusions and recommendations
WMA is a chance for the asphalt industry to enhance its product
performance, construction efficiency and environmental
management.
Conventional tests have demonstrated the increased stiffness
and improved temperature susceptibility of WMA additive involv-
ing bitumen samples. Storage stability tests have shown that nat-
ural zeolite involving bitumen samples, yield similar
performance compared to other additives. In terms of conventional
bitumen tests, chemical WMA additive exhibits more storage sta-
bility characteristics than other WMA additives.
Brookfield viscosity tests indicated that the addition of WMA
additives reduces the mixing and compaction temperature, thus
increases the workability of asphalt.
251
Detailed investigation performed by DSR test at low and high
frequency level and at different temperatures indicated that, the
complex modulus value increases with increase in frequency and
decreasing temperature. Increment in G is attributed to improved
elastic behavior of the sample. In terms of G values, no significant
variation is achieved in synthetic zeolite additive for G values and
in case of natural zeolite, 5% can be accepted as optimum WMA
content. Besides, 3% organic additive and 2% chemical additive
can also be considered as optimum additive contents.
The effect of WMA addition is also evaluated by the modifica-
tion indices. According to data obtained from MI values, 6% natural
zeolite WMA involving bitumen exhibits superior performance at
low (simulating heavy traffic conditions) and high frequency and
at all temperature levels.
In the light of findings from MI values, it is possible to consider
that the utilization of 5% of synthetic zeolite is suitable under hea-
vy traffic conditions (low frequency) and at high temperature
(above 60 °C).
In terms of MI values, significant improvement is achieved with
3% and above organic WMA additives. A clear distinction between
the low and high frequency levels of chemical WMA additive indi-
cates that 3% additive exhibits the highest MI value at low fre-
quency level.
It can also be considered that natural zeolite can be used as an
alternative WMA additive to synthetic zeolite.
This study covers the performance of WMA additives within the
base bitumen. The bitumen samples involving WMA additives to-
gether with aggregates should be investigated to evaluate the
effectiveness of WMA additives within the bitumen-aggregate
system.
Acknowledgements
This research was sponsored by the Scientific and Technical Re-
search Council of Turkey (TUBITAK) under the project number
110M567 for which the authors are greatly indebted. Besides, this
study has been carried out with the valuable contribution of Dokuz
Eylul University, The Graduate School of Natural and Applied
Sciences.
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