Construction and Building Materials 161 (2018) 175–185

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Construction and Building Materials

journal homepage: www.elsevier.com/locate/conbuildmat

Investigation of rheological properties of light colored synthetic asphalt

binders containing different polymer modifiers
Ping Tang, Liantong Mo ⇑, Changluan Pan, Hao Fang, Barugahare Javilla, Martin Riara
State Key Lab of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China

h i g h l i g h t s

Colored asphalt is prepared by means of synthetic resin.

Combination of SBS, EVA and PE Polymer is used for modification.

Rheological properties confirm the modification effect of various polymers.

Colored asphalt is susceptible to low temperatures and PAV aging.

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

Article history: Light colored synthetic asphalt (LCSA) binders were prepared by using aromatic oil, petroleum resin and
Received 27 July 2017 various polymer modifiers. The polymers used included styrene-butadiene-styrene block copolymers
Received in revised form 12 November 2017 (SBS), ethylene-vinyl acetate copolymer (EVA) and polyethylene (PE). The modification effects of single
Accepted 17 November 2017
and combined polymers were investigated. Fluorescence microscopy analysis confirmed the well disper-
sion of polymer phase and the compatibility of the binder. Fundamental research into rheological behav-
iors was conducted by using viscosity test, dynamic shear rheological test and bending beam test. Test
Keywords:
results showed that LCSA had a high viscosity at construction temperatures and strong frequency/tem-
Light colored synthetic asphalt (LCSA)
Polymer modifier
perature dependence on rheological properties. Polymer modification was identified by the master
Microstructure curves of phase angle and rheological black diagrams. BBR results demonstrated that LCSA binders were
Rheological property susceptible to low temperature and aging. Data analysis indicated that LCSA binders prepared by using
SBS, EVA and the combination of SBS plus EVA showed considerable performance for practical
application.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction
Roads and pavements are usually paved with asphalt concrete
or cement concrete. The application of asphalt concrete results in
a black pavement surface, or a grey-white surface for cement con-
crete. The combination of black and grey-white pavement surfaces
is colorless [1]. The increasing demand for colorful life requires
that some roads and pavements are covered with colored surfaces.
Therefore, colored pavements have become popular for the pur-
pose of beautifying parks, residential areas and scenic routes. In
some cities, specific colored lanes are designed for buses, bicycles
and pedestrians in order to improve transport safety and smooth-
⇑ Corresponding author at: Room 517, Concrete Building, State Key Laboratory of
Silicate Materials for Architectures, Wuhan University of Technology, Luoshi Lu 122,
Wuhan 430070, China.
E-mail address: molt@whut.edu.cn (L. Mo).
ness [2–6]. Compared with black asphalt pavements, cool colored
pavements are beneficial in reducing urban heat effect [7,8].
Colored pavements mainly consist of colored coating, colored
cement concrete and colored asphalt concrete. Among them, the
colored coating offers a wide variety of material and color. Adhe-
sive binders including epoxy, acrylic and polyurethane resin are
widely used to paste a thin colored coating on an existing pave-
ment surface [9]. Colored cement concrete pavements make use
of white cement and various pigments to create colored surfaces
[10]. Colored asphalt is an artificial light colored binder which
could be mixed with various pigments, additives and aggregates
to produce colored asphalt mixtures [3,11]. Colored asphalt mix-
ture were designed and constructed in a manner similar to conven-
tional asphalt mixture [12]. This indicated that light colored
asphalt should have a viscosity-temperature characteristic that
similar to traditional black asphalts at mixing and compaction
temperatures. In general, colored asphalt binder can be prepared

https://doi.org/10.1016/j.conbuildmat.2017.11.098
0950-0618/Ó 2017 Elsevier Ltd. All rights reserved.
176 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
in two ways; one is black color removal from asphalt and the other
is light-colored synthetic resin binder prepared by using oil refin-
ing residue, petroleum resin and polymer modifiers. Colored
asphalt is widely prepared by the light-colored synthetic method
because of the convenience and easiness of this production method
[11,13]. Aromatic oil and petroleum resin were used as the main
raw materials for the preparation of light colored asphalt. Sticky
aromatic oil could acted as fluxing medium to reduce viscosity at
production and construction temperature, while petroleum resin
contributed to hardness. The addition of petroleum resin was
reported to be a high amount of 35–50%, which could resulted in
increased softening point and viscosity, but reduced ductility as
well flexibility at low temperatures [13]. Polymer modifiers com-
monly used for asphalt modification were also available for light
colored synthetic asphalt (LCSA) binders. Polymer modifiers
formed network structure in LCSA binder and thus significantly
influenced the performance at both high and low temperatures
[13,14]. Munera reported that the optimum polymer content could
be determined by the flexibility and compatibility of modified
asphalt binder [15]. LCSA binder was shown to be sensitive to
aging, which destroyed the colloidal structure and thus deterio-
rated its performance. Ultraviolet light could result in color fading
in colored asphalt containing various pigments. Compared with
green colored asphalt mixture, red colored asphalt mixture had
better fading resistance [16,17]. Previous results obtained from
Marshall test, wheel tracking test and raveling test showed that
the performance of colored asphalt mixtures was comparable with
traditional asphalt mixture and has been successfully paved on
roads [18–20]. However, field inspection found that color fading
and loose of aggregate was the main distress for colored asphalt
pavements in Hubei province, China.
Colored asphalt pavements are increasingly applied to beautify
the environment and improve driving safety. Previous studies
mainly focused on the mixture design and construction technology
of colored asphalt mixture. Limited studies were done on the rhe-
ological properties of LCSA binders containing various polymer
modifiers. This paper aimed to get a fundamental understanding
on the rheological properties of LCSA binders prepared by synthetic
method. Aromatic oil, petroleum resin and polymer modifiers (SBS,
EVA and PE) were used as raw materials. Modification effects of
single and combined polymers were considered. For the purpose
of comparison, base asphalt and SBS modified asphalt were
employed. Fluorescence microscopy analysis was carried out to
examine the state of polymer dispersion. Detailed rheological
investigation was performed by means of dynamic shear rheome-
ter (DSR) and bending beam rheometer. The obtained results
would be used as a guideline for the development and optimiza-
tion of LCSA binders.
2. Experimental part
2.1. Raw materials and binder preparation
In this paper, light colored synthetic asphalt (LCSA) binders
were prepared by using aromatic oil and petroleum resin blended
with various polymer modifiers including SBS, EVA and PE. The
content of aromatic hydrocarbon of the aromatic oil employed
was 78% according to ASTM D2140. Its kinematic viscosity at
100 °C was 20 mm2/s tested in accordance with ASTM D445. The
used petroleum resin had a relative molecular weight ranging from
1000 to 2500 measured by Gel Permeation Chromatography (GPC)
and its softening point was between 80 °C and 90 °C determined by
ASTM E 28 Ring & Ball Method. SBS polymer that used in this study
is a linear type containing 30% styrene content with a molecular
weight of 105000. The value of melt flow index (MFI, ASTM
D1238) and vinyl acetic content (VA, ASTM-D5594) of EVA used
in this study were 50.1 g/10 min and 17.5%, respectively. Linear
low-density polyethylene (LDPE) was used and it had a Vicat soft-
ening point (ASTM D1525) of 89 °C.
Among the raw materials mentioned above, aromatic oil is a
sticky liquid with a very low softening point. It plays as a fluxing
medium for other raw materials. It also helps to reduce the viscos-
ity at production and construction temperature as well as to
improve the compatibility of mixed binder. Petroleum resin is a
brittle solid but can be softened and melted at high temperatures.
As cooled down it contributes to hardness. The addition of polymer
could improve the thermal stability at high temperatures and the
flexibility at low temperatures. Previous study done by Xi indicated
that polymer content of 7% together with resin content of 45% was
economical to prepared colored asphalt binders. Jin reported two
colored asphalt binders with polymer content 5% and 7% plus
polyester fibre 3%. High polymer content was used to improve
the rutting resistance of colored asphalt mixtures [14]. Table 1
gives the detailed information on the materials compositions of
various LCSA binders. In total, Eight LCSA binders were prepared
in laboratory. These asphalt binders were labeled A0 to A7. The test
program was designed to investigate the effects of single polymer
as well as the combined effects of two and three types of polymer
modifiers on the rheological properties. For this reason, the
amounts of aromatic oil and petroleum resin were constant as
52% and 40%, respectively for each binder, while polymer content
varied with the polymer type and the content of combined poly-
mers. High content of single polymer modifier and combined
two/three polymers was considered to form a continuous polymer
phase in LCSA binder. Among these eight LCSA binder, A0 was the
control sample that only consisted of aromatic oil and petroleum
resin without polymer modification. A1, A2 and A3 were prepared
by the addition of 8% SBS, 8% EVA and 8% PE, respectively. For A4,
A5 and A6, the combinations of 4.5% SBS plus 3.5% EVA, 4.5% SBS
plus 3.5% PE and 4.5% EVA plus 3.5% PE were considered, respec-
tively. Finally, A7 was prepared by considering the combination
of 3% SBS, 2% EVA plus 2% PE.
In this study, all of these LCSA binders were prepared by a sim-
ilar method of melting at high temperature and shear blending at
high speed. Aromatic oil was first heated to 180 °C in an oil-bath
heating container. Various polymers were added into aromatic oil
slowly and blended until completely melt and well dispersed using
a mix equipment (ESR-500, made by Shanghai ELE Co., Ltd., China)
with a shear blending speed of 4000 rpm for 45 min. Petroleum
resin was finally added and shear blended at a speed of 3000
rpm for 15 min.
For the purpose of comparison with these prepared LCSA bin-
ders, two commercial road paving asphalt binders, one base
asphalt binder and one SBS modified asphalt binders with 4.5%
SBS content were used as a reference. The base asphalt and SBS
modified asphalt were commonly used for hot-mix asphalt pave-
ments in Hubei province, China. The base asphalt had a penetration
of 67 dmm at 25 °C, a softening point of 47 °C and ductility at 15 °C
larger than100 cm. The properties of the SBS modified asphalt were
following: penetration of 54 dmm at 25 °C, softening point of 76 °C
and ductility of 52.1 cm at 5 °C.
2.2. Test methods
Differential scanning calorimetry (DSC) analysis (TG-DSC,
model STA449C, made by NETZSCH GmbH, Germany) was per-
formed to get insight into the thermal stability and melting point
of SBS, EVA, PE and petroleum resin. The sample of about 10 mg
was heated from room temperature to 600 °C at a heating rate of
10 °C/min under nitrogen condition supporting with a flowing
nitrogen of 20 ml/min.
 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185 177

Table 1
Materials composition of various LCSA binders.

No. Aromatic oil SBS EVA PE Petroleum resin

A0 52 – – 40
A1 52 8 – – 40
A2 52 – 8 – 40
A3 52 – – 8 40
A4 52 4.5 3.5 – 40
A5 52 4.5 – 3.5 40
A6 52 – 4.5 3.5 40
A7 52 3 2 2 40

The LCSA binders were subjected to the following conventional
binder tests: penetration (ASTM D5), softening point (ASTM D36),
ductility (ASTM D113) and rotational viscosity. The Brookfield Vis-
cometer with a temperature control system was implemented to
determine the viscosity of various LCSA binders in accordance with
ASTM D4402 [21]. The test temperatures ranged from 115 °C to
185 °C in order to investigate the viscosity at mixing and com-
paction temperatures.
Fluorescence microscopy was used to determine the dispersion
status of polymer modifiers within LCSA binders as well as to eval-
uate the nature of microscopic interactions among different poly-
mers [22,23]. The test sample was frozen at 20 °C and then
broken to obtain a relative smooth fracture surface. The obtained
fracture surface was observed by an optical microscope made by
Nanjing Jiangnan Novel Optics Co., Ltd of China (Model BM 2100)
with a magnification of 100 and 400 at ambient temperature.
A dynamic shear rheometer (DSR, MCR-101, made in Germany)
was used to characterize the rheological properties of LCSA bin-
ders. DSR tests were carried out in strain control and a small strain
level for each temperature was selected to ensure in the linear
region based on previous machine calibration testing. In order to
construct the master curve, frequency sweep testing was per-
formed at different temperatures ranging from 10 °C to 60 °C
with an interval of 10 °C. For each test temperature, the test fre-
quency ranged from 0.02 Hz to 64 Hz. The parallel plates of DSR
testing with a diameter of 8 mm plus 2 mm gap were used at a
low-temperature range from 10 °C to 20 °C, while 25 mm parallel
plates plus 1 mm gap for the high-temperature range between 30
°C and 60 °C. The rheological parameters including the phase angle
(d) and the complex modulus (G⁄) obtained from the DSR testing
were used as output for data analysis. By means of the time-
temperature superposition principle (TTSP), the d and G⁄data
obtained from different temperatures were horizontally shifted
to the reference temperature of 30 °C to form the master curves
[24].
Bending beam test was implemented by a bending beam
rheometer (Model TE-BBR, made by Cannon instrument company)
to investigate the rheological properties of these eight LCSA bin-
ders at low temperatures. Before BBR test, all of LCSA binders were
firstly subjected to RTFOT short-term aging and then long-term
aging conducted by Pressure Aging Vessel (PAV). The test condi-
tions of PAV aging were set at a pressure of 2.1 ± 0.1 MPa and a
temperature of 100 °C according to T0630, JTG E20-2011 [21]. In
this study, the BBR test was conducted in accordance with ASTM
D6648 standard test specification [25]. The creep stiffness S(t) at
60 s and the m-value representing the rate of stiffness changes ver-
sus time was analyzed. The mean values of S(t) and m were deter-
mined from three test samples for each asphalt binders. The BBR
test was carried out at low temperatures of 6 °C and 12 °C.
3. Results and discussion
3.1. DSC analysis results
Fig. 1 presents the DSC curves for SBS, EVA, PE and petroleum
resin. It should be noted that the melting point of a polymer is usu-
ally determined by the top of the endothermic peak. Considering
that the actual application temperature of asphalt binders is lower
than 200 °C, only the part of DSC curves below 200 °C is of interest.
One can see that the sharp peaks due to polymer melting occur for
EVA, PE and petroleum resin except for SBS. Based on the peak
temperature as indicated in Fig. 1, the melting point can be
determined as 80.2 °C, 105.32 °C and 72.3 °C for EVA, PE and
petroleum resin, respectively. Lower melting point indicates their

Fig. 1. DSC curves for SBS, EVA, PE and petroleum resin.

178 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
convenience for mixing and processing. SBS polymer does not
show any remarkable peak when temperature below 200 °C, which
implies that SBS polymer does not melt at a blending temperature
of 180 °C. High shear blending became thus necessary to reduce
the size of SBS polymer particles and promote their dispersion.
Fig. 2 shows the curves obtained from differential thermal analysis
(DTA) and thermogravimetric analysis (TG). It indicates that SBS,
EVA and PE shows a fair thermal stability on lose of mass at tem-
perature lower than 200 °C. However, petroleum resin shows a vis-
ible lose of mass at temperature above 150 °C, which indicates a
relatively poor thermal stability.
3.2. Conventional test results
Figs. 3–5 present the conventional test results, which included
penetration, softening point and ductility done on various LCSA
binders. In general, these three parameters are widely used to eval-
uate the basic engineering properties of an asphalt binder. Among
them, the penetration grade is widely used to characterize the
hardness and viscosity of asphalt binder, the softening point eval-
uates the high-temperature stability of asphalt binder, while the
ductility evaluates the low-temperature properties. An asphalt bin-
der with considerable penetration, high softening point and large
ductility is usually desired. According to Chinese specification of
CJJ/T218-2014, the penetration should range from 40 to 100
dmm depending on the binder grade. According to the specifica-
tion the minimum value of softening point is 52 °C for carriageway,
and 45 °Cfor the sidewalk and bicycle lanes [26]. With respect to
ductility, a minimum of 100 cm is desired. It can be seen that the
control LCSA binder A0 without any polymer has very poor ductil-
Fig. 2. DTA and TG curves for SBS, EVA, PE and petroleum resin (DTA: solid lines; TG: dashed lines).
Fig. 3. Penetration test results of various binders.
ity. After the inclusion of polymer, a significant improvement on
ductility can be observed. By comparing the data obtained from
A1, A2 and A3, one can see that SBS modifier shows the best mod-
ification effects, followed by EVA. The addition of PE shows the
worst modification, indicated by relatively low values of penetra-
tion, softening point and ductility. Such an asphalt binder may
have a bad applicability for both high and low temperature. In
comparison with SBS polymer, EVA shows an acceptable modifica-
tion effect. The only limitation of EVA modification is relatively low
ductility.
The combination effect of two types of polymer can be seen
from test results done on A4, A5 and A6. It is observed that A4 with
4.5% SBS plus 3.5% EVA shows a best effect, followed by A5 contain-
ing 4.5% SBS plus 3.5% PE. A6 prepared by using 4.5% EVA plus 3.5%
PE shows a worst drawback on the improvement of softening point
and ductility. The combination of these three types of polymer
used in A7 shows comparable results. The above analysis indicates
that SBS polymer have the most significant modification effect. PE
doesn’t have a positive effect and thus is limited for use. EVA could
provide a considerable improvement on the overall properties for
LCSA binders [27]. The combination of SBS plus EVA could be inter-
esting for low cost considerations. It can be concluded that the
modification effect on LCSA binder strongly depends on the elas-
tomer and plastomer nature of the used polymers.
3.3. Viscosity analysis
Fig. 6 presents the viscosity test results of various LCSA binders.
As can be seen, the viscosity of all the LCSA binders shows strong
temperature dependency. Increasing temperature results in
 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185 179

Fig. 4. Softening points of various binders.

Fig. 5. Ductility results at 15 °C of various binders except for SBS modified asphalt done at 5 °C.

Fig. 6. Viscosity-temperature curves of various LCSA binders.

significant reduction on binder viscosity. The viscosity is usually an
effective indicator for the asphalt binder’s workability. For hot mix
asphalt, the mixing and compaction temperature are usually deter-
mined by the viscosity-temperature curve [21]. For example, the
mixing temperature is determined by the temperature when the
viscosity equals to 0.17 ± 0.02 Pas, while the temperature that
reduces the viscosity to 0.28 ± 0.02 Pas is considered as com-
paction temperature. Based the viscosity-temperature curves plot-
ted in Fig. 6, one can determine that the mixing and compaction
temperatures for base asphalt are about 158 °C and 150 °C, respec-
tively. With respect to SBS modified asphalt, these two tempera-
tures can be higher than 180 °C, which is too high and is not in
agreement with the practical application of hot mix asphalt.
According to Chinese specification JTG F40-2004, the mixing tem-
perature of polymer modified asphalt has a maximum of 175 °C.
This also shows the limitation of the determination of construction
temperatures on the basis of asphalt viscosity. In general, A0 shows
a very low viscosity, while the addition of various polymers obvi-
ously increases the viscosity. A2, A6 and A7 show a trend on viscos-
ity change that is similar to the one of base asphalt. However, the
rest four LCSA binders show high viscosity, which is close to the
one of SBS modified asphalt. When only considering the modifica-
tion effect of single polymer among A1, A2 and A3, it is observed
that EVA had the lowest viscosity, followed by PE and then SBS.
The reason for the relatively low viscosity may be explain by the
difference of melting point of these three polymers as discussed
in Fig. 1. As a result, the existence of EVA with lower melting point
significantly reduces the viscosity of A4 and A6 which containing
SBS plus EVA and EVA plus PE. EVA with low melting point is of
interest because it provides an advantage on easy melting and
180 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
reduced viscosity at construction temperatures. Yuliestyan
reported that EVA modified asphalt with both improved in-
service properties and reduced application temperature can be
obtained by balancing VA content and MFI [26]. This indicates that
EVA has a promising use for the preparation of LCSA binder. The
viscosity results show that the prepared LCSA binders tend to have
high viscosity close to traditional SBS modified asphalt and thus
the construction temperatures could be referred to those of SBS
modified asphalt. The viscosity of some LCSA binders is higher than
that of SBS control binder at high temperatures due to the use of 8%
polymers. By reducing the amount of polymer used it will be pos-
sible to reduce the viscosity and the cost of the solutions. EVA can
reduce viscosity, but its melting point can also bring some prob-
lems if compaction temperatures are very low.
3.4. Fluorescence microscopy analysis
Fig. 7 shows the microstructures and morphologies of the LCSA
binders based on fluorescence microscopy analysis. For the pur-
pose of comparison, the image of SBS modified asphalt is also
given, in which the SBS modifier appears light green. A0 without
any polymer exhibits a green image, which indicates that petro-
leum resin is easy to blend homogeneously in aromatic oil. The
similar images can be observed on A1 with SBS and A2 with EVA.
Fig. 7. Fluorescence microscopy analysis of various LCSA binders.
For the images of A3 containing PE, discrete PE particles are
observed as circular shapes. Compared with traditional SBS modi-
fied asphalt, the existence of large amount of aromatic oil pro-
motes the dispersion and swelling of SBS modifier in LCSA binder
and thus a homogeneous system is obtained. EVA shows the good
dispersion, which agrees with Yuliestyan’s study. Yuliestyan
reported that EVA modified asphalt had a highly dispersed polymer
phase and very homogeneous binary at micro scale [26]. Generally,
SBS shows a better dispersion than PE because of its good compat-
ibility with aromatic oil [28,29]. The images of A4–A7 indicate that
SBS and EVA is a good combination to achieve well dispersion,
while PE particles are well indentified in various polymer combina-
tions. From the above analysis, it was concluded that EVA has an
excellent dispersion and the combination of SBS plus EVA is
optional.
3.5. Rheological master curves and black diagrams
The frequency dependence of complex modulus and phase
angle for the LCSA binders is presented in Figs. 8 and 9 by using
rheological master curves. These master curves are constructed
based on the time-temperature superposition principle (TTSP).
Consequently, the master curves provide insight into the viscoelas-
tic properties of the LCSA binders over a wide range of temperature
 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
and loading frequency, which are of special importance for the pre-
diction of road performance. In this study, the reference tempera-
ture is selected at 30 °C. Test data at other temperatures were
manually performed the horizontal shift to data at 30 °C to obtain
a smooth curve. The shift factors at various temperatures are
described by using the Arrhenius Equation [30].
  
Ea 1 1
aðTÞ0 ¼ exp  ð1Þ
R T T0
where: aðTÞ0 is the shift factor relative to the reference tempera-
ture; Ea is the activation energy, J/mol; R = 8.314 J/(molK); T is
the test temperature, K; T0 is the reference temperature, K.
The activation energy is determined by fitting the shift factors
using the method of least squares. Table 2 lists the fitting results
of the Arrhenius equation for all the binders. As can be seen, A0
without polymer has the highest value of activation energy close
to 240 kJ/mol. After adding polymer, the value reduces and ranges
from around 165 to 210 kJ/mol for the rest seven LCSA binders,
indicating the reduction on temperature susceptibility. These val-
ues are in agreement with the results reported by Ruan [31]. In
Ruan’s research, the activation energy of various asphalt binders
was found around 170–200 kJ/mol. This implies that LCSA binders
with polymer modification had similar temperature susceptibility
when compared with traditional base and SBS modified asphalt
binders.
It is known that the rheological properties of asphalt vary sig-
nificantly depending on type of asphalt and modification [32]. In
general, the complex modulus master curves of LCSA binders show
slightly different tends over a wide range of reduced frequency.
The addition of polymer tends to reduce the complex modulus at
Fig. 8. Master curves of complex modulus for LCSA binders at the reference temperature of 30 °C.
181
high frequency (low temperature range), but increase the complex
modulus at high frequency range (high temperature range). Com-
pared to conventional base asphalt and SBS modified asphalt, LCSA
binders with polymer show a marked increase in the complex
modulus at both high frequency range and low reduced frequency.
The increased complex modulus at high temperatures is good for
rutting resistance. However, higher complex modulus at low tem-
peratures is not desired since it may increase the risk of the brittle
facture [32].
When using base bitumen and A0 as the reference, the modifi-
cation effect of various polymers on LCSA binders is observed obvi-
ously. Among these three types of polymer, A3 with PE shows a
similar monotonous change with base asphalt, while other two
LCSA binders with SBS and EVA have complex curves, which are
similar to the one of SBS modified asphalt. This clearly indicates
that a polymer network doesn’t form in A3. It also is proved by
the low value of softening point of A3. Compared with base asphalt
and SBS modified asphalt, LCSA binders have lower values of phase
angle at high frequencies (low temperature range), which indicates
that they are relatively more stiff and brittle and thus have a higher
risk of brittle facture.
Among these asphalt binders, A4, A5, and A6 contain two types
of polymer modifiers, while A7 is the combination of three types of
polymer modifiers including SBS, EVA and PE. In Fig. 8, the combi-
nation effect of two or three types of polymer on complex modulus
can’t be well distinguished, especially at the high range of reduced
frequencies (low temperatures). At low range of reduced frequency
(high temperatures), a slight difference can be observed for A4 and
A5 since they have a relatively high complex modulus. This indi-
cates that the presence of SBS within the polymer combination
182 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
Fig. 9. Master curves of phase angle for LCSA binders at the reference temperature of 30 °C.
Table 2
the values of activation energy for various asphalt binders.
No. Ea (kJ/mol)
A0 238.34
A1 184.30
A2 207.28
A3 195.26
A4 168.08
A5 166.57
A6 189.28
A7 181.46
Base asphalt 181.65
SBS modified asphalt 197.06
plays a more effective role on high-temperature properties. It can
be concluded that the combination of different polymer modifiers
only result in a slight change of complex modulus over a wide
range of frequency.
With respect to the master curves of phase angle as shown in
Fig. 9, the effects of polymer addition are distinct at low frequen-
cies, but not at high frequencies. It is observed that A1, A4 and
A5 follow the similar shape over a wide range of reduced fre-
quency. This indicates the prominent effect of SBS modifier. By
comparing A3, A4 and A6, one can see that the effect of PE is rela-
tive weak since the addition of the other polymer modifier SBS or
EVA can change the trend obviously. The combination of three
types of polymers doesn’t give a positive effect when compared
to A1 that contains only SBS modifier.
Fig. 10 shows the black diagrams of various LCSA binders. The
black diagrams are obtained by plotting the measured complex
modulus against phase in a semi-logarithmic scale. In these dia-
grams, the values represented on the right and lower part indi-
cated by higher phase angles and lower complex modulus are
related to more viscous/soft binders that tested at high tempera-
tures. In contrast, the values shown on the left and upper part
showed by lower phase angles and higher complex modulus are
related to more elastic/hard binders tested at low temperatures
[33]. It can be seen that the curves of LCSA binders deviate obvi-
ously from those of traditional base asphalt and SBS modified
asphalt. This mainly results from the particular behavior of aro-
matic oil and petroleum resin blending. The changes of the curves
clearly distinguish the effects of polymer modification on LCSA bin-
ders. The monotonic decline on complex modulus with increasing
phase angle indicates a poor polymer modification as indicated by
R2 A3. However, a complex shape contributes to the strong modifica-
0.9946
tion effect exhibited by A4. The difference between peak and valley
0.9823 values is relatively larger when SBS polymer is included, indicating
0.9757 the excellent effect of modification for SBS polymer [33]. The
0.9850 results on black diagrams further confirm that SBS plus EVA is a
0.9815
good combination.
0.9898
0.9857
0.9807 3.6. BBR test results
0.9947
0.9958
Figs. 11 and 12 present the BBR test results of various LCSA bin-
ders at temperatures of 6 °C and 12 °C, respectively. Before BBR
test, the sample was subjected to RTFOT short-term aging and PAV
long-term aging. Creep stiffness and m-value are selected to eval-
uate asphalt binder’s ability to resist cracking at low temperatures
after aging. In general, the risk of thermal cracking is controlled by
low creep stiffness together with high m-value. According to SHRP
Superpave specification, asphalt binders after PAV long-term aging
should have a creep stiffness smaller than 300 MPa together with
m-value larger than 0.3 to release thermal stress [25]. As showed
in Figs. 11 and 12, the prepared LCSA binders are susceptible to
the reduction of temperature and PAV aging. PAV aging and tem-
perature reduction results in higher creep modulus, while lower
m-value indicates the declining resistance to thermal cracking.
Effects of PAV aging seem to be more significant when compared
with the temperature reduction from 6 °C to 12 °C.
When comparing with SBS modified asphalt, the prepared LCSA
binders tend to have higher creep modulus. This is in agreement
with the measurement results on complete modulus obtained from
DSR testing. It indicates that LCSA binders are harder than SBS
modified asphalt. When considering the effect of single polymer
modifier among A1, A2 and A3, it is found that A3 containing only
PE is the worst since it has the highest creep modulus and the low-
est m-value. The combination of polymer modifiers does not pro-
vide an obvious change on creep stiffness and m-value. However,
the existence of SBS is of benefit to EVA and PE.
When the test temperature is 6 °C, the creep stiffness of all
asphalt binders after RTFOT aging is lower than 300 MPa together
with m-value higher than 0.3. After PAV aging, the values of stiff-
ness sharply increased above 300 MPa except for A1.On the con-
trary, m-value drops obviously below 0.3 excluding A1. Further
 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185 183

Fig. 10. Rheological black diagrams of light various light colored asphalt binders.

Fig. 11. Creep stiffness for various asphalt binders at temperatures of 6° C and 12 °C.

Fig. 12. m-values for various asphalt binders at temperatures of 6 °C and 12 °C.
184 P. Tang et al. / Construction and Building Materials 161 (2018) 175–185
reducing temperature from 6 °C to 12 °C leads to higher creep
stiffness, but lower m-value. The above analysis indicates that
low-temperature performance of the studied LCSA binders is not
comparable with traditional SBS modified asphalt. It implies that
thermal cracking would be a risk for the prepared light colored
asphalt used in cold areas. Improvement of low-temperature prop-
erties could be expected by the addition of SBS. The use of SBS was
very effective to improve the flexibility at low temperatures. How-
ever, the large amount of SBS used also resulted in higher creep
modulus when compared with traditional SBS modified bitumen.
It thus would be important to reduce polymer content for the ben-
efit of reducing the creep modulus as well as the costs. Since pet-
roleum resin is hard and brittle, reducing the content of
petroleum resin or a relative soft alternative could be optional.
4. Conclusions
LCSA binders were prepared by using aromatic oil, petroleum
resin and various polymer modifiers. The related rheological prop-
erties of the obtained binders were analyzed and compared with
traditional base asphalt and SBS modified asphalt. Based on the
data obtained and the analysis presented in this paper, the follow-
ing conclusions can be drawn:
(1) DSC-TG analysis results showed that EVA and PE polymers
had low melting points, while SBS polymer did not show a
melting point as temperature below 200 °C. Fluorescence
microscopy analysis confirmed that melting point did not
directly relate to the dispersion state of polymer. SBS and
EVA dispersed homogeneously, but PE showed large discrete
particles.
(2) LCSA binders tended to have a high viscosity at construction
temperatures due to the addition of high polymer content.
DSR rheological properties showed strong frequency/temper-
ature dependence. The effect of polymer modification was
well identified by the master curves of phase angle and rheo-
logical black diagrams. In general, the ACSA binders exhibited
a particular rheological behavior, which deviated from those
of conventional base asphalt and SBS modified asphalt.
(3) BBR test results demonstrated that the low-temperature
performance of LCSA binders were susceptible to the reduc-
tion of temperature and PAV aging. The risk of thermal
cracking should be considered for the application in cold
areas. This limitation indicates that further improvement
on low-temperature properties is needed.
(4) The modification effect on LCSA binder strongly depends on
the elastomer and plastomer nature of the used polymers.
SBS polymer was the most effective modifier, followed by
EVA and PE. The combination of SBS plus EVA could be
optional to reduce the cost and the difficulty of asphalt
preparation process. Petroleum resin is hard and brittle,
reducing the content of petroleum resin or a relative soft
alternative could be optional to improve the flexibility at
low temperatures.
(5) This study was limited to use high contents of petroleum
resin and polymers. This resulted in high viscosity, creep
stiffness and cost. The contents of the mentioned materials
could be further optimized by considering the requirements
on the binder properties as well as the cost.
Acknowledgements
Financial support from the National Natural Science Foundation
of China (No. U1733121) and the China Scholarship Council is
acknowledged. The authors are grateful for the cooperation
between the People’s Republic of China and the Government of
Kenya and Uganda and express their desire to see a prolonged
and stronger cooperation between the two states.
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