Polymer Testing 21 (2002) 633640

www.elsevier.com/locate/polytest
Product Performance
Improved properties of polystyrene-modified asphalt through
dynamic vulcanization
a,*
Hailong Jin , Guangtao Gao a, Yong Zhang a, Yinxi Zhang a, Kang Sun b,
Yongzhong Fan b
a
Polymeric Materials Research Institute, Shanghai Jiao Tong University, Shanghai 200240, Peoples Republic of China
b
State Key Lab of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200030, Peoples Republic of China

Received 27 September 2001; accepted 7 November 2001

Abstract

Storage-stable polystyrene (PS)-modified asphalt has been successfully prepared in the presence of linear styrene
butadienestyrene triblock copolymer (SBS) through dynamic vulcanization. The vulcanization characteristics of the
asphalt/PS/SBS/sulfur blends were studied using a strain-controlled rheometer. At temperatures from 140 to 180C,
the curing rate of the blends increases significantly with increasing temperature. A suitable processing temperature is
between 170 and 180C for the sake of good mechanical and thermal stability properties. The physical properties,
including softening point, penetration, and ductility at low temperature of the modified asphalt through dynamic vulcan-
ization were compared to that of modified asphalt without sulfur. The storage stability of the PS-modified asphalt was
effectively improved in the presence of SBS through dynamic vulcanization. The morphology and rheological properties
of the modified asphalt were also investigated using an optical microscope and a dynamic shear rheometer, respectively.
The morphology was compared between the pure PS-modified asphalt, the PS/SBS-modified asphalt, and the
PS/SBS/sulfur-modified asphalt, which indicated that the compatibility and high-temperature storage stability of the
PS-modified asphalt were improved significantly in the presence of SBS through dynamic vulcanization. 2002
Elsevier Science Ltd. All rights reserved.

Keywords: Modified asphalt; Dynamic vulcanization; Storage stability

1. Introduction separation under quiescent conditions at elevated tem-

It is well known that polymer modified asphalt (PMA)
has been used in road technology with the intention of
reducing road deterioration such as rutting, cracking and
stripping [1]. There are a large variety of polymers cur-
rently being used as PMA, such as styrenebutadiene
styrene triblock copolymer (SBS), styrenebutadiene
rubber (SBR) and polyethylene (PE). However, the
major obstacle to widespread usage of PMAs in paving
practice has been their tendency towards gross phase
* Corresponding author. Tel.: +86-21-5474-3265; fax: +86-
21-5474-1297.
E-mail address: jhl003@mail1.sjtu.edu.cn (H. Jin).
peratures because of the poor compatibility between
polymer and asphalt [2].
Polystyrene (PS) is one of the most commonly used
thermoplastic polymers, and generates a considerable
amount of recoverable scrap material [3]. Due to its stiff-
ness over a range of service temperatures, PS would also
seem very suitable for modification of asphalt and could
thereby effectively contribute to its stiffness and
strength. However, PS has been found to be very difficult
to disperse into asphalt even using high shear because
of its incompatibility with asphalt. Consequently, the
coarsely dispersed phase separates quickly once agitation
stops. Thus it is necessary to improve the storage stab-
ility of PS-modified asphalt for practical use, which is
focused on by only one publication [4].

0142-9418/02/$ - see front matter 2002 Elsevier Science Ltd. All rights reserved.
PII: S 0 1 4 2 - 9 4 1 8 ( 0 1 ) 0 0 1 3 5 - 0
634 H. Jin et al. / Polymer Testing 21 (2002) 633640
In our opinion [5], the preparation of storage-stable
PMA with sulfur reported by a number of patents [68]
is the process of dynamic vulcanization and this concept
can be applied in practice. Dynamic vulcanization, which
is widely used in rubber/plastic blends, is a route to new
thermoplastic elastomers that have properties (such as
ultimate mechanical properties, stability of phase mor-
phology in the melt, and so on) as good or even, in some
cases, better than those of elastomeric block copolymers
[9]. Dynamic vulcanization can be described as follows:
after sufficient melt mixing of rubber and plastic, e.g.,
in an internal mixer or a compounding extruder (to form
a well-mixed blend), vulcanizing agents are added. Vul-
canization then occurs while mixing continues. Fine vul-
canized rubber particles, which are formed by shearing
and shattering, are dispersed homogenously in a continu-
ous plastic phase. As for the processing procedure, the
preparation of PMA with sulfur is similar to dynamic
vulcanization of rubber/plastic blends.
Storage-stable SBS-modified asphalt was prepared
through dynamic vulcanization in our laboratory and
Wen et al. investigated its rheological properties [10].
On the basis of this, we considered that PS could be
stabilized in asphalt emulsion in the presence of SBS to
exhibit a two-phase morphology consisting of glassy PS
domains connected together by rubber polybutadiene
(PB) segments.
In this paper, storage-stable PS-modified asphalt is
reported. The objective of the present work is to identify
the existence of the vulcanization of
asphalt/PS/SBS/sulfur blend, to investigate and explain
the rheological behavior of PS-modified asphalt in the
presence of SBS before and after dynamic vulcanization,
and also to verify its morphology visually using
optical microscopy.
2. Experimental
2.1. Materials
Asphalt, AH-70 paving asphalt was obtained from
Zhongyou Xingneng Asphalt Factory of Jiangyin,
Jiangsu, China. The physical properties of this asphalt
are as follows: penetration: 70 dmm (25C, ASTM stan-
dard D5); softening point: 47.0C (ASTM standard
D36).
PS, grade 158K, was provided by Yangzi-BASF styr-
enics Co., Ltd, China.
SBS, grade 1301, was produced by Yanshan Petro-
chemical Co., Ltd., China. SBS 1301 is a linear polymer
containing 30 wt% of styrene, Mw=110,000.
The sulfur used was an industrial grade product, made
in Shanghai Jinghai Chemical Co., China
2.2. Preparation of PMA
Asphalt was heated to 160C in a small container until
it flowed fully. PS and SBS (the amounts were based on
100 parts asphalt except especially stated) were mixed
into the asphalt under high-speed stirring for 60 min and
the PS/SBS/asphalt blend became essentially homogen-
ous. Subsequently, a level of sulfur was incorporated into
the blend at high stirring speed for 90 min at 180C.
2.3. Measurement of vulcanization characteristics
Asphalt was heated to 160C in a small container until
it flowed fully (similar to the preparation of PMA
above); 4.0 parts of PS and 4.0 parts of SBS were mixed
into the asphalt under high-speed stirring for 60 min.
When the temperature of the blend was reduced to below
120C, 0.4 parts of sulfur was added to the blend and
the stirring continued for 15 min at low speed so as to
ensure unreacted, homogenous blends were obtained.
Below 120C, neither the reaction between asphalt and
sulfur nor the vulcanization of the SBS/sulfur blend
would take place according to the literature [11].
A strain-controlled rheometer, Advanced Rheology
Expanded System (ARES) of Rheometric Scientific Co.,
USA, with cup and plate geometry was used to deter-
mine the vulcanization characteristics of the blends. A
2.0 g sample was put in the lower cup (30 mm in
diameter). After the sample was heated until it flowed,
the upper parallel plate (25 mm in diameter) was lowered
to contact tightly with the sample. All the samples were
held at a constant temperature of 80C for 10 min, then
heated rapidly to a given temperature, 120, 140, 160,
180C, respectively, and kept there for 1 h. The applied
frequency was 50 rad/s.
The maximum torque, MH, the minimum torque, ML,
t0, t50, t90, and curing rate, 1/t50, were obtained from the
curing curves. t0 is the time when the torque is equal to
ML. t50 and t90 are the times when the torque is equal to
(MHML)50%+ML and (MHML)90%+ML, respect-
ively.
2.4. Measurement of physical properties and storage
stability
The physical properties of asphalts, including soften-
ing point, penetration and ductility, were measured in
accordance with ASTM D36, D5 and Chinese specifi-
cation GB/T 4508, respectively.
The storage stability of modified asphalts was meas-
ured as follows: the sample was put into an aluminum
foil tube, 32 mm in diameter and 160 mm in height.
The tube was sealed without an air enclosure, and stored
vertically in an oven at 163C. After 48 h the tube con-
taining the modified asphalt was cooled to ambient tem-
perature and cut horizontally into three equal parts. The
 H. Jin et al. / Polymer Testing 21 (2002) 633640
upper and lower parts were then melted and stored in
separate small cans labeled T and B, respectively. The
softening points of T and B materials were determined.
If the difference of the softening points between T and
B is less than 2.5C, the sample can be regarded to have
good storage stability.
2.5. Rheological characterization
The ARES rheometer with parallel plate geometry (25
mm in diameter) was used to determine the rheological
characteristics of the PMA. A temperature sweep was
applied over the range 30100C at a fixed frequency of
10 rad/s and variable strain. The strain was chosen to be
as small as possible to ensure measurement in the linear
region, but large enough to allow sufficient torque read-
ings. A sample of about 1.0 g was put onto the lower
plate. After the sample was heated to become molten,
the upper parallel plate was lowered to contact tightly
with the sample and trimmed. The final gap was adjusted
to 1.2 mm. All the samples were held at a defined, con-
stant temperature for 10 min, then the temperature was
varied in 2C increments. Various viscoelastic para-
meters, such as G*, G, G1/2, and tan d were collected
automatically by the RSI Orchestrator software.
2.6. Morphology observation
A 510 mg asphalt sample was heated and slowly
pressed between two glass slides and the sample mor-
phology was observed using an optical microscope
(made by Leica Co., Germany) with a hot plate. Mor-
phology changes as a function of time were monitored
at a magnification of 400 at 160C.
3. Results and discussion
3.1. Vulcanization characteristics
In our experiment to study the vulcanization character-
istics of the asphalt/PS/SBS/sulfur blends, all the asphalt
blends were kept at 180C and the changes in torque
with time are compared among asphalt/sulfur (100/0.4),
asphalt/PS/SBS (100/4.0/4.0) and asphalt/PS/SBS/sulfur
(100/4.0/4.0/0.4) blends as shown in Fig. 1. The torque
of the asphalt/sulfur blend is the lowest and the torque
of the asphalt/PS/SBS/sulfur blend is the highest. There
is little dependence of the torque on time for the
asphalt/sulfur blend, which indicates that the reaction
between asphalt and sulfur has little effect on the torque
at low levels of sulfur. A great amount of sulfur (up to
50 wt% in asphalt) can improve the physical and mech-
anical properties of the sulfur/asphalt mixture [11],
which is attributed to a reaction between asphalt and sul-
fur. The reaction was confirmed to start at about 130C
635
Fig. 1. Comparison of the vulcanization of the blends.
by Filippis et al. [12]. However, the small amount of
sulfur (only 0.4 wt% in asphalt) used in this study cannot
modify asphalt individually, and its novel modification
effect can only be achieved through the reaction between
sulfur and SBS. Moreover, the torque of the
asphalt/PS/SBS blend is higher than the torque of the
asphalt/sulfur blend. The torque kept constant with
increasing time, which is in accord with our expectation
and implies that chemical reaction of the asphalt/PS/SBS
blend is nearly impossible. The torque of the
asphalt/PS/SBS/sulfur blend increases significantly with
increasing time, which indicates that a vulcanization
reaction occurred in the blend, and reflects the process
of gradual formation of elastic crosslinking networks.
In our study, the vulcanization of the
asphalt/PS/SBS/sulfur blend was observed to begin at
120C, and to change to decomposition and degradation
of the blend above 220C. The torquetime curves of the
blend at different temperatures ranging from 120 to
180C are shown in Fig. 2. As can be seen, the vulcaniz-
ation of the blend depends on temperature to a great
extent. At 120C, the torque has little change with time,
implying that there is no obvious vulcanization reaction
at this temperature. The blends were found to vulcanize
dramatically at temperatures from 140 to 180C,
especially at 160C, which gave the greatest variation
in torque.
Some important vulcanization parameters such as MH,
ML, t0, t50 and t90 from the torquetime curves of Fig. 2
at temperatures from 140 to 180C are given in Table 1.
It can be seen that with increasing temperature, MH, ML,
t0, t50 and t90 of the blends decrease, while curing rate
increases. Curing rate increases significantly at elevated
temperature 160180C. Therefore, the PS/SBS-modi-
fied asphalt in the presence of sulfur should be processed
at a relatively high temperature such as 160180C.
636 H. Jin et al. / Polymer Testing 21 (2002) 633640

Fig. 2. Effect of temperature on the vulcanization of the Fig. 3. Effect of PS content on the vulcanization of the
asphalt/PS/SBS/sulfur (100/4/4/0.4) blend. asphalt/PS/SBS/sulfur blend.

asphalts (the pure PS-modified asphalt and the PS/SBS-

Table 1 modified asphalt) are given together. As can be seen
Vulcanization parameters of PS/SBS (4.0/4.0) modified asphalt
from Fig. 4(a), with increasing PS content the softening
Temperature (C)
point of the pure PS-modified asphalts increases, which
implies that high temperature properties of asphalt would
140 160 180 be improved by PS. When the content of SBS is fixed
at 3 wt%, the PS/SBS-modified asphalts show higher
MH (g cm) 6.73 6.29 4.67 softening point compared with the pure PS-modified
ML (g cm) 5.48 2.92 1.61 asphalts having the same PS content. The effect on
MHML (g cm) 1.25 3.37 3.06 softening point of increasing the PS content has a similar
t0 (min) 10.30 8.55 6.30 tendency to that of the pure PS-modified asphalts.
t50 (min) 38.05 26.50 12.05 Through dynamic vulcanization, the softening point of
t90 (min) 56.57 40.85 39.80
the PS/SBS/sulfur-modified asphalt is significantly pro-
Cure rate (100 2.63 3.77 8.29
min1)
moted compared with the other two asphalts at the same
PS content. The softening point of the asphalt is dramati-
cally promoted when the PS content is lower than 3 wt%,
while it slightly increases when PS content is more than
Moreover, as indicated from the curing curves, the pro- 3 wt%. Fig. 4(b) shows that, as PS content increases, the
cessing of the blend can be completed in 1 h. penetrations of the three modified asphalts decrease, and
Fig. 3 shows the effect of PS content on vulcanization the PS/SBS/sulfur-modified asphalts show the most dra-
characteristics of the PS/SBS/sulfur blend, and the vul- matic change. Fig. 4(c) shows that the low-temperature
canization parameters are also given in Table 2. It can be ductility of the pure PS-modified asphalt is smallest, and
seen that with increasing PS content, MH and ML increase the ductility of the PS/SBS/sulfur-modified asphalt is
significantly due to enhanced viscosity. With changing significantly promoted. With increasing PS content, the
PS content, the cure rate changes slightly because the ductility of the modified asphalts shows no evident
blends have the same SBS and sulfur content and the change.
vulcanization just takes place between the SBS and the Compared to the large differences in the top and bot-
sulfur. tom sections of the PS/SBS-modified asphalts (Fig. 5),
the differences for the PS/SBS/sulfur-modified asphalts
3.2. Physical properties and storage stability are not more than 1.5C when the PS/SBS ratio is not
more than 1:1. This indicates that the storage stability of
The effect of PS content on the physical properties PS-modified asphalt is effectively improved. It can be
and storage stability of the PS-modified asphalt is shown seen that when the PS/SBS ratio is more than 1/1, the
in Figs. 4 and 5, respectively. To investigate the novel difference of the PS/SBS/sulfur-modified asphalts is just
improvement of the properties of the PS/SBS/sulfur- over 2.5C, which may be attributed to the insufficient
modified asphalts, the results of the other corresponding coverage of butadienerubber, thus leading to slight
 H. Jin et al. / Polymer Testing 21 (2002) 633640
Table 2
Effect of PS content on vulcanization characteristics of PS/SBS1301 modified asphalt
PS content (wt%)
0 2
MH (g cm) 1.38
ML (g cm) 0.46
MHML (g cm) 0.92
t0 (min) 6.30
t50 (min) 11.80
t90 (min) 36.30
Cure rate (100 min1) 8.47
phase separation of the samples. Hence, it can be con-
cluded that with suitable content of PS/SBS and sulfur,
storage-stable PS-modified asphalt can be achieved in
the presence of SBS through dynamic vulcanization.
3.3. Rheological properties
Asphalt may exhibit either elastic or viscous behavior,
or a combination of both, depending on the temperature
and the time over which the asphalt is observed. Poly-
mers may modify asphalt rheology by virtue of their high
molecular weights, chain entanglements and polymer
asphalt interactions (physical or chemical). This modifi-
cation may be demonstrated by dynamic mechanical
analysis.
For rutting resistance at high temperatures, increased
complex modulus (G*) and elastic modulus (G) and low
tangent phase angle (tan d) values are favorable because
they reflect a more elastic behavior [13]. Fig. 6 shows
the effect of PS content on rheological properties of the
PS/SBS-modified asphalt. It can be seen that G* of the
original asphalt decreases sharply with increasing tem-
perature and is very low at high temperature, while tan
d of the original asphalt dramatically increases at the
same time. At a temperature of 100C, the phase angle
(d) of the original asphalt approaches 90. In this case,
the stored energy per cycle of deformation becomes neg-
ligible compared to that dissipated as heat, so at this time
asphalt exhibits nearly pure viscous liquid behaviour
without any elasticity. As the PS content increases, the
G* of the modified asphalts increases at high tempera-
ture. Its change becomes apparent when the PS content
is over 3.0 wt% in the presence of 3 wt% SBS, which
is probably attributed to a continuous physical network
formed throughout the asphalt matrix.
Fig. 7 shows the effect of PS content on the rheolog-
ical properties of the PS/SBS/sulfur-modified asphalt
through dynamic vulcanization. It can be seen that the
addition of sulfur leads to smaller changes in tan d with
increasing temperature than for the modified asphalts
without sulfur. The change in tan d of 3.0 wt% SBS
637
4 6
2.01 4.67 5.22
0.73 1.60 2.53
1.28 3.07 2.69
6.80 6.30 6.05
11.95 12.05 12.57
31.3 39.80 39.55
8.37 8.29 7.95
modified asphalt is less than 12 at temperatures from 30
to 100C, and with addition of the PS, the tan d value
of the PS/SBS/sulfur-modified asphalt at high tempera-
ture is much lower (less than 9). As the PS content
increases, tan d of the modified asphalts changes less
with increasing temperature. G* of the modified asphalts
increases significantly with increase in PS content. This
phenomenon can be related to the formation of a chemi-
cal network structure by vulcanization.
The Strategic Highway Research Program (SHRP)
adopted the temperature of the modified asphalts when
G*/sin d is equal to 1 kPa as a criterion for the high-
temperature performance of asphalt [14]. The results are
shown in Table 3. It is found that the modified asphalts
through dynamic vulcanization have a higher perform-
ance grade than the corresponding modified asphalt with-
out sulfur. As the PS content increases, the performance
grade of the modified asphalt was greatly promoted
through dynamic vulcanization, which appears much
more obvious when compared with the modified asphalt
without sulfur.
3.4. Morphology
The compatibility between polymer and asphalt is
critical to the properties of PMAs [15]. The morphology
of PMAs is usually investigated using an optical micro-
scope by characterizing the distribution and the fineness
of polymer in the asphalt matrix. Fig. 8 shows the orig-
inal micrographs of the PS-modified asphalts on a hot
plate at 160C. The original micrograph of pure 3 wt%
PS-modified asphalt is shown in Fig. 8(a), and it can be
seen that the white PS particles are dispersed in the
asphalt matrix (appears black) coarsely, which implies
that PS is difficult to disperse into asphalt even using
high shear stress, perhaps because of the intrinsic struc-
tural features of rigid molecular chains with high melt
strength. The original micrograph of the
PS/SBS(3.0/3.0)-modified asphalt is shown in Fig. 8(b),
and it can be seen that the size of PS particles becomes
smaller with the incorporation of SBS, which indicates
638 H. Jin et al. / Polymer Testing 21 (2002) 633640

Fig. 5. Effect of PS content on storage stability of the PS-

modified asphalts: (a) the PS/SBS-modified asphalt; (b) the
PS/SBS/sulfur-modified asphalt.

that SBS can promote a uniform dispersion of PS in the

Fig. 4. Effect of PS content on physical properties of the PS-
modified asphalts.
asphalt matrix. The original micrograph of the
PS/SBS/sulfur (3.0/3.0/0.15) modified asphalt is shown
in Fig. 8(c), and it can be seen that the size of PS par-
ticles becomes dramatically smaller so that it nearly
approaches the resolving power of the microscope at a
magnification of 400. Fig. 9 shows the micrographs of
the PS-modified asphalts on the hot plate at 160C for
2 h. It can be seen that the particles of the pure 3 wt%
PS-modified asphalt appear to coalescence and their size
becomes large as shown in Fig. 9(a), which implies that
the pure PS-modified asphalt has very poor high-tem-
perature storage stability. The micrograph of the
PS/SBS(3.0/3.0)-modified asphalt on the hot plate at
160C for 2 h is shown in Fig. 9(b). It can be seen that
the PS particle size increases gradually with time, which
indicates that the polystyrene domain of SBS, which acts
as a receiving unit for stabilization of the dispersed PS
 H. Jin et al. / Polymer Testing 21 (2002) 633640 639

Fig. 8. The original micrographs of the PS-modified asphalts

on the hot plate at 160C: (a) pure 3 wt% PS-modified asphalt;
(b) PS/SBS(3.0/3.0)-modified asphalt; (c) PS/SBS/sulfur
(3.0/3.0/0.15)-modified asphalt.

Fig. 6. Effect of PS content on theological properties of the

PS/SBS-modified asphalts.

Fig. 9. Micrographs of the PS-modified asphalts on the hot

plate at 160C for 2 h: (a) pure 3 wt% PS-modified asphalt; (b)
PS/SBS(3.0/3.0)-modified asphalt.

particles, is dispersed finely throughout the asphalt while

Fig. 7. Effect of PS content on theological properties of the
PS/SBS/sulfur-modified asphalts.
without being stabilized in the asphalt matrix. The micro-
graph of the PS/SBS/sulfur (3.0/3.0/0.15) modified
asphalt on the hot plate at 160C for 2 h shows there
has been no change. This means that the compatibility
of PS/SBS-modified asphalt has been improved signifi-
cantly through dynamic vulcanization. Hence, this blend
can be stored at elevated temperature.

4. Conclusions
Table 3
Effect of PS content on the performance grade of the PS modi-
Storage-stable PS-modified asphalt has been success-
fied asphalts fully prepared in the presence of SBS through dynamic
vulcanization. The vulcanization characteristics of
PS content SBS content Temperature when G*/sin asphalt/PS/SBS/sulfur blend can be determined by an
d=1 kPa (C) ARES strain-controlled rheometer. The physical proper-
ties of the PS-modified asphalt, including softening
Before adding After adding point, penetration and ductility, can be characterized.
sulfur sulfur The softening point increases significantly and the pen-
etration reduces when sulfur is present. The storage stab-
0.0 0.0 63.6
ility can be effectively improved through dynamic vul-
0.0 3.0 67.2 73.0
3.0 3.0 70.3 79.5 canization. The rheological properties of the PS/SBS-
6.0 3.0 72.3 82.1 modified asphalt and the PS/SBS/sulfur-modified asphalt
can be characterized by using the strain-controlled rhe-
ometer. The addition of sulfur to the modified asphalt
640 H. Jin et al. / Polymer Testing 21 (2002) 633640
results in the formation of a chemical vulcanized net-
work structure in the asphalt matrix, and the high tem-
perature performance of the modified asphalts can be
improved and their temperature susceptibility is reduced
to a great content. PS content has a great effect on the
rheological properties of the asphalts. Morphology
observation confirms that the compatibility and storage
stability of the PS-modified asphalt can be improved in
the presence of SBS through dynamic vulcanization.
Acknowledgement
The authors acknowledge the financial support pro-
vided by the National Natural Science Foundation of
China, whose registered number is 59973011.
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