Construction and Building Materials 215 (2019) 823–838

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Construction and Building Materials

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

Analysis of mechanism and time-temperature equivalent effects of

asphalt binder in short-term aging
Wanli Ye a,b, Wei Jiang a,b,⇑, Pengfei Li a,b, Dongdong Yuan a,b, Jinhuan Shan a,b, Jingjing Xiao a,c
a
School of Highway, Chang’an University, South 2nd Ring Road Middle Section, Xi’an, PR China
b
Key Laboratory for Special Area Highway Engineering of Ministry of Education, Chang’an University, South 2nd Ring Road Middle Section, Xi’an, PR China
c
School of Civil Engineering, Chang’an University, South 2nd Ring Road Middle Section, Xi’an, PR China

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

Rheological properties were tested for

asphalt aged under different
situations.

Chemical methods (FT-IR and GPC)
were tested for asphalt aged under
different situations.

The characteristics of rheological
properties under different aging
conditions were analyzed.

A time-temperature equivalent
model of short-term aging was
constructed.

Relationships between rheological
properties and chemical composition
were obtained.

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

Article history: The degradation of asphalt pavement performance is severely affected by the aging of asphalt. In order to
Received 26 November 2018 improve the anti-aging performance of asphalt, it is necessary to study the aging mechanism of asphalt
Received in revised form 4 March 2019 first. The objective of this paper was to systematically study the characteristics and mechanism of short-
Accepted 24 April 2019
term aging of neat asphalt based on rheological indexes and chemical indexes, including complex mod-
Available online 3 May 2019
ulus (G*), phase angle (d), stiffness (S), m-value, fatigue performance parameter (Nf), carbonyl index (IC@O)
and polydispersity (PDI). The short-term aging of asphalt was performed by the rolling thin film oven test
Keywords:
(RTFOT) at different temperatures and durations, the rheological properties were evaluated by the
Asphalt
Short-term aging
dynamic shear rheometer (DSR) and bending beam rheometer (BBR), the chemical indexes were got by
Time-temperature equivalent effect the Fourier transform infrared (FT-IR) and the gel permeation chromatography (GPC). Meanwhile, the
Rheological properties time-temperature equivalent effects based on the high/low-temperature performance of asphalt were
Chemical properties analyzed. The relationships between asphalt rheological properties and chemical indexes were discussed.
Correlation analysis The results showed that the fatigue resistance was most sensitive to aging while compared with the high/
low-temperature performance of asphalt. The indexes including G*, S, and Nf tended to increase as the
aging degree increased, whereas other rheological indexes had opposite trends. According to the chang-
ing characteristics of the high/low-temperature performance of asphalt, a time-temperature equivalent
effect model of asphalt aging was constructed. Moreover, both the oxidation and volatilization of asphalt
components were accelerated as the aging temperature increased, but the volatilization was more sen-
sitive to temperature than the oxidation. Based on the correlation analysis, both IC@O and PDI exhibited

⇑ Corresponding author.
E-mail address: jiangwei@chd.edu.cn (W. Jiang).

https://doi.org/10.1016/j.conbuildmat.2019.04.197
0950-0618/Ó 2019 Elsevier Ltd. All rights reserved.
824 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838
a strong correlation to rheological properties. Therefore, prediction models based on IC@O and PDI were
constructed to predict the rheological properties of aged asphalt.
1. Introduction
With the development of the transportation industry around
the world, the asphalt pavement has been widely used [1], such
as the airfield and the high-grade road pavement [2], for its advan-
tages of a smooth surface, no seams, low vibration, low noise, short
construction period and easy maintenance [3–5]. Moreover, the
asphalt, as an adhesive material [6–10], is composed of asphalte-
nes, resins, aromatics, and saturates [11]. The asphaltene and
resins content were proved had a great influence on the asphalt
viscosity, and the temperature susceptibility of asphalt decreased
as the asphaltene increased [12]. Therefore, the rheological proper-
ties of asphalt, which was related to viscosity, have been proved
that could be used to determine the performance of the pavement
directly [13–16].
Aging of asphalt, occurred during the production, transportation,
mixing and throughout its whole service life, is a very complex pro-
cess [17], which is influenced by the environment and traffic inten-
sity [1]. The aging of asphalt, which makes the asphalt becomes stiff
and brittle [14,18–20] and the pavement vulnerable to damage
[21–23], is an essential cause for road performance degradation
[24,25]. According to the Superpave binder specifications and other
studies, aging is divided into three stages [26,27]: (a) before mixing,
(b) hot mix asphalt (HMA) production and construction (short-term
aging) [28,29], and (c) whole service life (long-term aging) [30–33].
Many scholars have studied aging and have come up with some
causes of aging: (a) oxidation [10,34],(b) ultraviolet irradiation
[25,35,36], (c) volatilization [37], and (d) condensation [38]. As for
the long-term aging, which was mainly caused by oxidation and
ultraviolet irradiation [39], it was also influenced by uncontrollable
factors such as atmosphere, temperature, sunlight, rain, and snow
[40,41]. In order to improve the anti-aging properties of asphalt,
modifiers such as SBS, SBR, and rubber were mainly used. However,
the uncontrollability of the factors affecting the long-term aging
made it difficult to conduct further researches. However, the heat-
ing temperature, heating duration, and heating environment in the
short-term aging of asphalt could have been artificially controlled
to prevent aging. Therefore, the short-term aging of asphalt should
be further studied.
Rolling thin film oven test (RTFOT), which has been applied by
AASHTO and ASTM, is one of the most common tests to simulate
the short-term aging [42,43] and have been widely used. However,
for the study of the aging mechanism, only 163 °C or 85 min is not
enough. On the one hand, the 163 °C was inherited from the tem-
perature of thin film oven test (TFOT) in 1963 [44], and can be
traced from the asphalt test temperature of Dow [45]. It has been
well known that the production and modification of asphalt have
undergone tremendous changes during the past 100-year period.
On the other hand, asphalt modified by polymers is more viscous
than the neat asphalt, and it could not flow sufficiently in the glass
bottle to achieve the aimed aging effect while under the standard
RTFOT settings. But this problem can be overcomed by adjusting
the temperature and duration of aging. Therefore, it is necessary
to discuss the short-term aging mechanism of asphalt by setting
a series of different aging configurations (temperature and dura-
tion) to determine the short-term aging settings applicable to dif-
ferent situations.
Based on the aging tests, the change of physical properties
[7,32,46–51], chemical properties [34,39,52–54], mechanical prop-
Ó 2019 Elsevier Ltd. All rights reserved.
erties [22,55,56], and rheological properties [7,9,10,20,57–66]
were proved correlate with the deterioration of asphalt perfor-
mances. However, previous asphalt tests such as penetration and
softening point were empirical experiments and cannot adequately
describe the viscoelastic characteristics of asphalt [25]. Thus, the
rheological experiments such as dynamic shear rheometer (DSR)
and bending beam rheometer (BBR) were introduced to evaluate
the rheological properties of asphalt [6]. Moreover, several studies
had been proved that there were strong correlations between rhe-
ological indexes and asphalt performances [67–69]. The DSR was
used to study the high-temperature performance, the middle-
temperature performance and the fatigue resistance of the asphalt
[6,9,66,70]. For example, Yut et al. [62] employed the DSR to study
the high-temperature performance indexes such as complex mod-
ulus and phase angle after aging by RTFOT and pressure aging ves-
sel (PAV). The results showed that the indexes had a strong
correlation with the viscoelasticity of asphalt. Liu et al. [71]
employed the DSR to study the aging properties of SBS modified
asphalt under through laboratory aging and field aging. According
to the dynamic response, they constructed a relationship between
the aging in the laboratory and in the field, which suggested that
the asphalt aged in the field for 22 years could be equal to the
asphalt aged in the laboratory for five days. However, as mentioned
earlier, different long-term aging conditions would lead to differ-
ent aging results, so the promotion of this conclusion was still open
to question. The BBR was used to study the low-temperature per-
formance of asphalt [11,25,72,73]. For example, Behnood et al. [6]
employed the BBR to study the effect of different types of modifiers
on the low-temperature performance of asphalt. The results
showed that modifiers would reduce the stiffness of asphalt, but
different modifiers had different influences on the m-value.
Besides, with the development of science and technology, a series
of chemical methods, such as the Fourier transform infrared (FT-IR)
and the gel permeation chromatography (GPC), were used to char-
acterize the composition characteristics of asphalt [1]. As for the
FT-IR, it can distinguish and classify asphalt based on their chem-
ical composition, mainly represented by peak positions, peak
heights and peak areas [65,74–76]. Tarsi et al. [77] studied the
effects of different aging methods on the functional groups of
asphalt. The results showed that different aging temperatures
would lead to different degrees of carbonyl formation. As for the
GPC, it can predict the viscosity changes [78–80] and molecular
weight distributions [2,81] of asphalt. Moreover, some relation-
ships between the FT-IR [82–84]/GPC [17,71,85,86]and the rheo-
logical properties have been discussed.
In conclusion, nowadays the asphalt aging is mainly discussed
based on the modified asphalt with different modifiers and differ-
ent modifier contents. Although modifiers, usually made of poly-
mers and were complex in composition, may have some
improvement in the anti-aging properties of asphalt, the mecha-
nism of the improvement is complicated to be proved. However,
the neat asphalt, although the compositions have a little different
from source to source, the reaction complexity in the aging process
is far less than the modified asphalt. Thus, it is more suitable for
the aging mechanism discussing.
However, there were few studies on the chemical composition
and rheological properties of neat asphalt under different aging
configurations. Therefore, the objective of this study was to sys-
tematically study the short-term aging process of the neat asphalt
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838
by RTFOT, the rheological test equipment such as DSR and BBR, and
the chemical equipment such as FT-IR and GPC. Moreover, the
time-temperature equivalent effects in the short-term aging pro-
cess and the relationships between asphalt rheological properties
and chemical compositions could be discussed further. What
should be noted is that this study not only lays the foundation
for the anti-aging researches of asphalt in the future but also pro-
vides useful guidance for the operation of the asphalt industry.
2. Materials and methodology
2.1. Materials
Bitumen A-70, which was bought from Shanxi great road indus-
trial Co., Ltd and produced by S-OIL corporation from South Korea,
was used in this study. The basic performance of the A-70 is pre-
sented in Tables 1. The 70 means that the penetration of that bitu-
men is between 60 and 80.
2.2. Methods
The research procedure is shown in Fig. 1, including aging the
bitumen under different configurations, testing the sample by the
two major rheometers (DSR and BBR), investigating the chemical
variations by the FT-IR and GPC. The processes of preparing the
aged samples are introduced in Section 2.2.1. The methods to eval-
uate the rheological properties are presented in Section 2.2.2 and
2.2.3. The methods to investigate chemical characteristics in the
aging process are shown in Sections 2.2.4 and 2.2.5.
2.2.1. Laboratory aging
The RTFOT has become one of the most commonly used test
methods to simulate the short-term aging of bitumen. According
to the ASTM D2872 standards, 35 g bitumen sample was first
placed in a glass bottle with a narrow top opening. Then the bottles
were rotated in the 163 °C oven at a rate of 15 rpm for 85 min with
the bottle opening facing a jet of air. The process of rolling spread
35 g bitumen into thin film with a thickness of 5  10 lm, making
the bitumen being aged efficiently and uniformly [87].
As the petroleum refining process improves, the content of
heavy components in the bitumen continues to increase. Moreover,
modifiers in the modified bitumen are usually composed of the
polymer, which increases the viscosity of bitumen while improving
the performance of asphalt. Thus, a higher temperature is required
to achieve the specified fluidity of bitumen. However, considering
the general maximum heating temperature when using bitumen
(190 °C), the limit temperature of the oven (200 °C) and the flash
point of the bitumen (usually 220 °C ～ 260 °C), the maximum
aging temperature of bitumen was set to 191 °C in this study.
Based on the analysis above, a series of aging temperatures and
a series of aging durations were set to investigate the time-
temperature equivalent effect and the aging mechanism. At each
duration and temperature, 8 bottles filled with bitumen partici-
Table 1
Properties of bitumen A-70.
Parameters Unit ASTM test method
Penetration (25 °C, 100 g, 5 s) 0.1 mm D5
Softening point °C D36
Ductility (15 °C, 5 cm/min) cm D113
Dynamic viscosity (60 °C) Pas D2493
Specific gravity g/cm3 D70
Flashpoint (Cleveland) °C D92
Solubility (trichloroethylene) % D2042
825
pated in the aging, 3 of which were used to calculate the mass
change, and the rest were used for subsequent tests, as shown in
Fig. 2. For the mass change test, the average of the three replicate
tests was taken as the final result.
2.2.2. Dynamic shear rheometer (DSR) test
The discovery hybrid rheometer HR-1 produced by TA instru-
ments from America was used to study the rheological properties
of aged and unaged bitumen. The number of replicate samples
used in the DSR test was one. However, repeated tests were per-
formed on several samples, and the deviations of repeated tests
were small since the excellent accuracy of the DSR. Therefore, in
this paper, no repeated samples were tested in the amplitude
sweep, the temperature sweep, and the linear amplitude sweep.
2.2.2.1. Amplitude sweep. The amplitude sweep was performed to
determine the linear viscoelastic (LEV) deformation limit of the
bitumen, and the result was shown in Fig. 3. Subsequent DSR tests
will be designed based on the LEV deformation limit.
2.2.2.2. Temperature sweep. Temperature sweep was performed
from 46 °C to 82 °C with steps of 6 °C. The strain amplitude was
controlled at 1.0%, and the angular frequency was controlled at
10 rad/s. Two plates with a diameter of 25 mm were used, and
the gap between parallel plates was 1 mm.
2.2.2.3. Linear Amplitude Sweep (LAS). For the time sweep took a
long time to characterize the fatigue resistance of bitumen [88],
the linear amplitude sweep was used as a substitute [89]. There
were two steps, and they were performed in succession. The first
was frequency sweep, which was designed to obtain information
on the rheological properties. The frequency sweep test was
employing an applied load of 0.1% strain over a range of frequen-
cies from 0.1  30 Hz. The second was amplitude sweep, which
was intended to measure the damage characteristics of the mate-
rial. The amplitude sweep was run at 25 °C and a frequency of
10 Hz. The loading scheme was increasing the strain from 0.1% to
30%. Two plates with a diameter of 8 mm were used, and the gap
between parallel plates was 2 mm [90,91]. The fatigue resistance
was then calculated from the results of frequency sweep and
amplitude sweep. According to AASHTO TP 101–12 (R2016), the
Nf is calculated by Eqs. (1)–(4) [92].
At first, the damage accumulation in the bitumen is calculated
by Eq. (1):
X
N a
DðtÞ ffi
1
½pc20 ðC i1  C i Þ1þa ðt i  t i1 Þ1þa ð1Þ
i¼1
where CðtÞ ¼ jG jðtÞ=jG jinitial , jG jðtÞ is complex modulus at time t
(MPa) and jG jinitial is the initial undamaged value of jG j (MPa); c0
is the applied strain (%); a ¼ 1=m, in which m come from the
best-fit line of logG0 ðxÞ ¼ mðlogxÞ þ b; t is the testing time (s).
For each data point at a given time t, the relationship between C
(t) and D(t) can be fit into Eq. (2):
C ðtÞ ¼ C 0  C 1 DðtÞC2 ð2Þ
where C0 = 1, C1, and C2 are curve-fit coefficients
Then the Df, which is the value of D(t) at failure, is calculated
corresponding to the maximum peak shear stress by Eq. (3):
Results
 1=C2
72 C 0  C at peak stress
Df ¼ ð3Þ
47 C1
>200
170 The fatigue performance parameter Nf now could be calculated
1.011 by Eq. (4):
303
99.5 Nf ¼ Aðcmax ÞB ð4Þ
826 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838

Fig. 1. The flow chart of the methodology.

Fig. 2. Laboratory short-term aging plan.

250000 low-temperature performance of bitumen. The deflection in the

G* middle of the beam under load is measured, and then the creep
stiffness (S) and m-value could be calculated. The lower S indicates
that bitumen has a stronger resistance to cracks and the higher m-
value indicates that bitumen has a greater ability to relax from the
200000 stress [6,95]. And the requirements of performance grading require
that the S should less than 300 MPa and m-value should larger than
G* (Pa)

0.3 after 60 s’ loading of BBR.

A previous study [73] showed that the trends of stiffness and m-
values had similar characteristics at different test temperatures.
150000 Besides, the increase in aging degree had no significant effects on
the changes in stiffness and m-value at 6 °C, and sometimes the
stiffness of aged bitumen could not meet the specification require-
ments at a test temperature of 18 °C and 24 °C. Thus, 12 °C
was chosen as the test temperature of BBR to study the low-
temperature performance under different aging configurations in
100000
0.01 0.1 1 10 100 this paper. The number of replicate samples used in the BBR test
Strain (%) was three, which could meet the requirements of the specifications
issued by ASTM/AASHTO. The average of three replicate tests was
Fig. 3. Linear viscoelastic (LVE) deformation limit of bitumen. used as the final result.

2.2.4. Fourier transform infrared (FT-IR) analysis

1þð1C 2 Þa
10D In order to investigate the effect of temperature and duration on
where A ¼ ð1þð1C f
pC 1 C 2 Þa , B ¼ 2a, and cmax is the maximum aging quantitatively, an aging index (usually based on carbonyl or
2 ÞaÞð

expected strain (%). sulphoxide) should be used to evaluate the aging degree
[34,52,53]. Existing researches had shown that carbonyl had better
2.2.3. Bending beam rheometer (BBR) test stability under high temperature than sulphoxide [96] and usually,
According to ASTM D2872 and ASTM D6648 [93,94], the change of sulphoxide was too small to be perceived in the
the BBR test, which usually conducted at low temperatures short-term aging [97]. Thus, the carbonyl index would be used to
(6 °C, 12 °C, 18 °C and 24 °C), is used to evaluate the determine the aging degree in this study. Besides, it has been
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838 827

proved in some studies that quantitative analysis using peak area 70

was more accurate than using peak height [62,98,99]. Therefore,
the carbonyl index calculated by peak area was used in this study. 60
Portable Fourier transform infrared spectrometer Thermo Sci-
entific Nicolet iS5 was used in the study. The wavenumber of 50

Response (mV)
recorded spectra ranges was from 650 cm1 to 4000 cm1 with
4 cm1 resolutions. The number of scanning was 32 times, and 40
the attenuated total reflectance (ATR) with crystal ZnSe was used
for the spectrum collection. Thermo Scientific OMNIC was adopted 30
as spectrum analysis software. Since the ATR can be automatically
locked after reaching the load threshold and bitumen has plasticity 20
at the room temperature, the ATR could extend different bitumen MMS
to a similar thickness when reaching the load threshold, which 10
provides a necessary precondition for the quantitative analysis LMS SMS
method of FT-IR [9]. For the quantitative analysis method, the area 0
between a baseline and the peak line could be measured, which is 14 15 16 17 18 19 20 21

shown in Fig. 4, and then the peak area ratios could be calculated. Elution time (min)
However, there is no uniform standard for quantitative analysis
Fig. 5. An example of the gel permeation spectrogram of bitumen.
by FT-IR on the aging degree of bitumen and different methods
were proposed by previous studies [9,62,75,100–103]. The most
common one was to use the ratio of the peak area at 1700 cm1 represented were the number of molecules that belongs to each
to the sum of the peak areas in the range of 2000 cm1 to size. Then the ratios of each size could be calculated. The number
650 cm1, which is shown by Eq. (5). The number of replicate sam- of replicate samples used in the GPC test was one. However,
ples used in the FT-IR test was three, and the average of three repli- repeated tests were performed on several samples. The deviations
cate tests was used as the final result. of repeated tests were small since the excellent accuracy of the
A1700 GPC. Therefore, in this paper, no repeated samples were tested in
IC¼O ¼ ð5Þ the GPC test.
A1700 þ A1600 þ A1450 þ A1375 þ A870 þ A815 þ A730
In order to study the characteristics of molecular weight distri-
where A1700 means the peak area of the spectral band at 1700 cm1, bution during the short-term aging [107], PDI could be calculated
A1600 means the peak area of the spectral band at 1600 cm1, and so based on Eqs. (6)–(9) [108]:
on. Pn
i¼1 wi M i
Mw ¼ Pn ð6Þ
i¼1 wi
2.2.5. Gel permeation chromatography (GPC) analysis
PL-GPC 50 Integrated GPC/SEC System from Agilent Technolo- Ni Mi
gies was used in this study and tetrahydrofuran (THF) was selected wi ¼ Pn ð7Þ
i¼1 N i M i
as mobile phase solvents in this study. The chromatogram of
molecular weight distribution could be obtained after 30 min. Pn
i¼1 N i M i
The curve was divided into 13 equal parts according to some pre- Mn ¼ Pn ð8Þ
i¼1 N i
vious studies [85,104–106], as shown in Fig. 5. It is defined that the
part 1  5 belong to the large molecular size (LMS), part 6  9
Mw
belong to the middle molecular size (MMS), and the rest belong PDI ¼ ð9Þ
Mn
to the small molecular size (SMS). What the areas under the curve
where Mn is the number average molecular weight and Mw is the
weight average molecular weight; Mi is the molecular mass, wi is
the weight fraction of each type of molecule, and Ni is the number
0.15 of molecules of Mi.
Above the indexes, Mn shows the statistical average molecular
weight of all the molecular in the sample. Compared to Mn, large
molecular weight components are taken into account in Mw, and
O3
the larger molecular weight the component, the more it con-
0.10 tributes to Mw. PDI is used to evaluate the molecular weight distri-
Absorbance

bution broadness of a sample, and the larger the PDI, the broader
the molecular weight [108].
Absorbance
peak area 3. Results and discussion
0.05
3.1. Effect of aging on bitumen performance

O2 3.1.1. High-temperature performance

The high-temperature performance of bitumen is evaluated by
O1 complex modulus and phase angle at 64 °C, which show the extent
0.00
1700 1600 1500 1400 1300 1200 1100 of elastic and viscous deformation of bitumen at a high tempera-
Wavenumber (cm ) -1 ture and is got from the temperature sweep as mentioned in Sec-
tion 2.2.2. As the aging duration increases, the log(G*) increases,
Fig. 4. Peak area calculation method. and there is a strong linear relationship between log(G*) and aging
828 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838

2.2
85
2.0

1.8 80

1.6
75
log(G*) (kPa)

1.4

(°)
1.2 70

1.0
65
0.8

0.6 60

0.4
55
50 100 150 200 250 300 350 400 50 100 150 200 250 300 350 400

Duration (min) Duration (min)

(a) log(G*) (b )
G* (kPa) (°)
84
190 106 190

93 81

185 185
80 78
°C
°C

67 180 75
180

54 71

175 175
41 68

170 28 170 65

15 62
165 165
3 58
100 150 200 250 300 350 100 150 200 250 300 350
Duration (min) Duration (min)
*
(c) Contour map of log(G ) (d) Contour map of
Fig. 6. High-temperature performance under different aging configurations.

duration, as shown in Fig. 6(a). Besides, as the aging temperature
increases, the slope of log(G*) increases gradually. This is because
the aging is accelerated by the increase of temperature. However,
the phase angle has an opposite tendency with complex modulus,
as shown in Fig. 6(b). As the aging duration increases, the d
decreases, and there is also a strong linear relationship between
d and aging duration. As the aging temperature increases, the slope
of d decreases gradually. Besides, it could be seen from Fig. 6(c) and
(d) that the complex modulus and phase angle changes slowly first
and then is accelerated, which means that the initial stage of short-
term aging has a fewer effect on the high-temperature perfor-
mance than the final stage.
3.1.2. Low-temperature performance
The low-temperature performance of bitumen is evaluated by
the creep stiffness (S) and m-value after 60 s’ loading of BBR.
According to Fig. 7(a), aging has a negative effect on low-
temperature performance, which also has been found in a previous
study [73]. However, two different trends of stiffness are found
while in different aging configurations. While under 163 °C and
170 °C, as the aging duration increases, stiffness first increases
rapidly, and then the rate of growth gradually slows down. But
while under 177 °C, 184 °C and 191 °C, the rate of growth does
not slow down. As for m-value, while under 163 °C and 170 °C,
as the aging duration increases, m-value first decreases rapidly,
and then the rate of decrease gradually slows down. But while
under 177 °C, 184 °C and 191 °C, the rate of decrease does not slow
down, as shown in Fig. 7(b). This may because only parts of the
light components could be volatilized at 163 °C or 170 °C. Though
the light components decrease as aging last, further aging duration
does not cause further volatilization when that parts of compo-
nents are completely volatilized. As the temperature increase,
more and more components could be volatilized, and a higher tem-
perature would lead to a higher volatilization speed.
It seems that the low-temperature performance under different
aging configurations has similar results with the high-temperature
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838 829

0.45 300

0.40 250
% (5)

S (MPa)
m

0.35 200

0.30 150

0.25 100

-50 0 50 100 150 200 250 300 350 400 -50 0 50 100 150 200 250 300 350 400
Duration (min) Duration (min)
(a) S (b) m-value
S (MPa) m
297 190 0.401
190

280 0.384

185 185
263 0.367
°C
°C

180 245 180 0.349

228 0.332

175 175
211 0.315

170 194 170 0.297

176 0.280

165 165
159 0.263
100 150 200 250 300 350 100 150 200 250 300 350
Duration (min) Duration (min)

(c) Contour map of S (d) Contour map of m-value

Fig. 7. Low-temperature performance under different aging configurations.

performance, but it should be noticed that the influence of the ini-
tial stage of short-term aging on the low-temperature performance
is more significant than on the high-temperature performance, as
shown in Fig. 7(c) and (d). Thus, it could be inferred that the
low-temperature performance is more sensitive to aging than the
high-temperature performance.
3.1.3. Fatigue resistance
The fatigue resistance of bitumen is evaluated by Nf under dif-
ferent maximum expected strains (cmax = 2.5%, cmax = 5%). Fig. 8
presents the Nf under different maximum expected strains and
aging configurations. The Nf (cmax = 2.5%) is larger than Nf
(cmax = 5%), but they seemed had a similar tendency. At each aging
temperature, as the duration increase, the Nf increases rapidly at
the beginning but is followed by a slower increase. As the temper-
ature increases, the slope of Nf increases gradually, which means
the aging is accelerated by the increase of temperature. This may
because as the temperature increases, more and more components
could be volatilized, and a higher temperature lead to a higher
volatilization speed. As the bitumen component volatilizes, the
bitumen becomes more and more viscous, resulting in an increase
in fatigue resistance. Besides, it could be seen from Fig. 8(c) and (d)
that there should be a time-temperature equivalent effect in the
fatigue resistance of bitumen during the short-term aging, which
is similar to the high-temperature performance and the low-
temperature performance of bitumen. According to the change
ratio of rheological properties in the initial stage of aging, as shown
in Figs. 6(c) and (d), 7(c) and (d), and 8(c) and (d), the fatigue resis-
tance is most sensitive to aging, followed by the low-temperature
performance, and the high-temperature performance is least sensi-
tive to aging.
3.2. Time-temperature equivalent effect
According to the rheological properties change characteristics
under different aging conditions, it can be inferred that there
would be a time-temperature equivalent relationship in the
short-term aging of bitumen base on the high/low-temperature
performance. Thus, the sigmoidal function is introduced to investi-
gate the performance conversion under different combinations of
830 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838

Fig. 8. Fatigue resistance of bitumen under different aging configurations.

aging durations and aging temperatures, which is implemented by 407957

logjG j ¼ 2:178 þ ð12Þ
Eq. (10). The master curve is constructed at 177 °C, as shown in 1 þ e21:1502:573 ðlogðtÞþaðTÞÞ
Fig. 9. The fitting results of the master curve of the high-
where G* is the complex modulus, d is the minimum modulus value,
temperature performance and the low-temperature performance
t is the aging duration under reference temperature, a represents
are listed in Eqs. (11) and (12), respectively. Besides, the changes
the span of modulus values, b and c are shape parameters, and a
of the shift factor (a(T)) under different temperature are shown
(T) is the shift factor.
in Fig. 10. As the aging temperature increases, the shift factor grad-
ually becomes larger, and the slope of the fitted line gradually
3.3. Aging mechanism analysis
increases, making the fitting function gradually shifts to the left.
This is because as the temperature increases, the aging process is
For the researches of bitumen aging, observing and summariz-
accelerated and the aging degree increases. Besides, there are
ing the time-temperature equivalent effect of rheological proper-
strong correlation coefficients in the time-temperature equivalent
ties of bitumen has significant meanings for engineering practice.
conversion model (larger than 0.92), which indicate that it may be
However, only when the mechanisms of bitumen aging are sys-
feasible to use the sigmoidal function to adjust the short-term
tematically studied by appropriate chemical analysis methods,
aging conditions of different bitumen.
the time-temperature equivalent effect of bitumen aging could
a be possible to be applied and generalized.
logjG j ¼ d þ ð10Þ
1 þ ebc ðlogðtÞþaðTÞÞ Therefore, the mass change, FT-IR, and GPC are chosen for the
chemical analysis of bitumen aging. In general, the mass change
3:323 could reflect the macroscopic changes of bitumen in the aging pro-
logjG j ¼ 0:345 þ ð11Þ
1 þ e10:6353:892 ðlogðtÞþaðTÞÞ cess, which would be discussed in 3.3.1. The FT-IR could reflect the
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838
Fig. 9. Time-temperature equivalent effect.
0.2
high-temperature performance
low-temperature performance
0.1
0.0
(T)
-0.1
-0.2
-0.3
163 170 177 184
°C
Fig. 10. The changes in shift factor under different temperature.
microscopic changes of the oxidation of components during the
aging process, which would be discussed in 3.3.2. The GPC could
reflect the migration of bitumen components during the aging pro-
cess, which would be discussed in 3.3.3. And the relationships
between index from FT-IR and index from GPC would be discussed
in 3.3.4.
3.3.1. Effect of aging on bitumen mass
Fig. 11 presents the mass change of bitumen under different
aging configurations. As the aging duration increases, the mass of
bitumen increases while under 163 °C, 170 °C and 177 °C, but
decreases while under 184 °C and 191 °C. And as the temperature
increases, the slope of the mass change curve decreases. This is
because of the aging of bitumen, which is generally considered to
be the result of a complex process, including chemical reactions
(oxidation, composition, decomposition) and physical changes
(volatilization). Oxidation, absorbing O2 into the bitumen, would
increase the mass of bitumen. Composition and decomposition of
831
191
Fig. 11. Mass change of bitumen under different aging configurations.
components would not affect the total mass of the bitumen.
Volatilization, volatilizing components out of bitumen, would
decrease the mass of bitumen. From the analysis above, it could
be concluded that the mass change of bitumen is mainly caused
by oxidation and volatilization. As the temperature increases, both
oxidation and volatilization are accelerated, but the effect of
volatilization on the bitumen mass significantly exceeds the effect
of oxidation on the bitumen mass, which means the volatilization
is more sensitive to temperature than the oxidation.
3.3.2. FT-IR analysis of different aging conditions
Fig. 12 presents the FT-IR spectra of bitumen after aging under
191 °C. It can be seen from Fig. 12 that as the aging duration pro-
longs, the peak area at 1700 cm1 gradually increase, indicating
that new carbonyl groups are continuously produced. However,
there are no significant changes in the peak area at 1030 cm1,
indicating that the content of sulfoxide is stable during the
short-term aging of bitumen. Therefore, it is more suitable to char-
acterize the aging degree with carbonyl in the short-term aging of
832 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838

Fig. 12. FT-IR spectra after aging at 191 and different duration.

Fig. 13. Standardized carbonyl index under different aging configurations.

bitumen. Since the carbonyl index calculated by the method men-
tioned above is small and is not suitable for comparison directly.
Therefore, the index is standardized to [0, 1] and dived into 10
levels, such as [0, 0.1], [0.1, 0.2] and so on, as shown in Fig. 13.
Fig. 13(a) presents the carbonyl index under different aging
configurations. While under 163 °C and 170 °C, the carbonyl index
has similar characteristics. As duration increase, the carbonyl index
first increases slowly, and then the growth is accelerated while
after aging for 265 min. The slope of the carbonyl index at
177 °C, 184 °C, and 191 °C is greater than the slope of the carbonyl
index at 163 °C and 170 °C. The reason is that the components in
bitumen are more active in a high-temperature environment, mak-
ing components easier to react with oxygen. At 163 °C and 170 °C,
the volatilization of the light components (Aromatics and Satu-
rates) [73] in the bitumen would carry away parts of energy in
the surface of the film, which hinders the oxidation. Besides, the
distribution of the carbonyl index in different aging configurations
is similar to the rheological properties of bitumen, as shown in
Fig. 13(b). Thus, it could be inferred that there would be correla-
tions between the carbonyl index and the rheological properties
of bitumen.
Fig. 14 presents the relationship between the carbonyl index
and the high-temperature performance. As the carbonyl index
increases, the complex modulus increases, the phase angle
decreases, the fatigue factor and rutting factor increases, which
means the high-temperature performance of bitumen has been
improved. Besides, there is a strong correlation between the car-
bonyl index and the high-temperature performance of bitumen.
It can be inferred that the increase of high-temperature perfor-
mance is mainly caused by the oxidation of bitumen components.
Thus, it is reasonable to predict the high-temperature performance
of bitumen by carbonyl index.
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838 833

Fig. 14. The relationship between the carbonyl index and high-temperature performance.

300 m=0.41342-0.23482Ic=o+0.0992I2c=o 0.45

R2=0.82282

0.40
250
S (MPa)

S
m

m
0.35
200

0.30
150
S=134.7254+152.2984Ic=o
0.25
R2=0.93658
100
0.0 0.2 0.4 0.6 0.8 1.0

IC=O

Fig. 15. The relationship between the carbonyl index and low-temperature
performance. Fig. 16. The relationship between the carbonyl index and fatigue resistance.

Fig. 15 presents the relationship between the carbonyl index
and the low-temperature performance. As the carbonyl index
increases, the stiffness of bitumen increases and the m-value
decreases. Besides, there is a strong correlation between the car-
bonyl index and the low-temperature performance of bitumen,
and the correlation coefficient between the stiffness and the car-
bonyl index is better than the correlation coefficient between the
m-value and the carbonyl index. It can be inferred that the
decrease of low-temperature performance is mainly caused by
the oxidation of bitumen components, but the ability to relax from
stress is also affected by other factors. However, it seems still fea-
sible to predict the low-temperature performance of bitumen by
the carbonyl index.
Fig. 16 presents the relationship between the carbonyl index
and fatigue resistance. It could be seen from the fitting results that
there is a good correlation between the carbonyl index and fatigue
resistance, which suggests the increase of fatigue resistance may
be caused by the oxidation of bitumen components. Thus, it seems
feasible to predict the fatigue resistance of bitumen by the car-
bonyl index.
3.3.3. GPC analysis of different aging configurations
As mentioned in 2.2.5, the peak area of the molecular weight
distribution indicates the number of molecules in the region, and
the more the number of molecules, the larger the peak area.
Fig. 17(a) presents the molecular weight distribution of the bitu-
men sample aged under 177 °C. It could be seen from the figure
that the components migrations caused by aging mainly occur in
MMS and LMS. Fig. 17(b)(f) presents the molecular weight distri-
butions of bitumen under different aging configurations. At each
aging temperature, as the duration increases, the SMS and MMS
decreases gradually, but the LMS increases gradually. It is because
the components of bitumen during aging are converting toward
the adjacent larger molecular size components, which means the
SMS is converted to the MMS and LMS, and the MMS is converted
to the LMS. For components like saturates, aromatics, resins, and
asphaltenes (SARA), the convert could be considered as that from
aromatics to resins, and from resins to asphaltenes [109]. However,
it should be noticed that when after experiencing a specific aging
duration, the SMS starts to increase rather than decrease, as shown
in Fig. 17(b)(f). The reason may because while the SMS and MMS
834 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838

70 @177
100
0 min 13% 12% SMS
16% 15% 13% 13% 14%
60 85 min MMS
145 min 80 LMS
Response (mV)

50 205 min
265 min

Content (%)
325 min 60
40 64% 64%
65% 64% 62%
385 min 67% 65%
30 40

20
20

10 MMS 20% 22% 23% 24% 24% 24%

17%
LMS SMS 0
0 0 85 145 205 265 325 385
13 14 15 16 17 18 19 20 21 Duration@163°C (min)
Elution time (min)

100 100
14% 13% 12% 12% 13% SMS 15% 14% 11% 12% SMS
16% 15% 16% 15% 15%
MMS MMS
80 LMS 80 LMS
Content (%)
Content (%)

60 60
63% 62% 61% 62% 61%
65% 64% 63% 63% 63%
67% 66% 67% 65%

40 40

20 20

23% 25% 26% 26% 22% 22% 23% 27% 27%

17% 19% 21% 17% 20%
0 0
0 85 145 205 265 325 385 0 85 145 205 265 325 385
Duration@170 (min) Duration@177 (min)

(c)170 (d)177
100 100
14% 14% 12% 13% SMS 13% 12% 13% 10% 11% 10% SMS
16% 15% 15% 16%
MMS MMS
80 LMS 80 LMS
Content (%)

Content (%)

60
59% 60 61% 59% 59%
61% 59% 58% 63% 61% 60%
63% 62%
67% 67%
40 40

20 20
27% 29% 29% 27% 27% 29% 29% 31%
22% 23% 25% 24%
17% 17%
0 0
0 85 145 205 265 325 385 0 85 145 205 265 325 385
Duration@184 (min) Duration@191 (min)

(e)184 (f)191
Fig. 17. The transformation process of molecular size caused by aging.

are still converting to LMS, the LMS is decomposing into the SMS has strong correlations with the rheological properties of bitumen
after absorbing too many smaller molecules. The results are consistent with the conclusions obtained above. On
Fig. 18 represents the relationships between the polydispersity the one hand, a part of saturates and aromatics is converted to
and the rheological properties. The PDI, calculated by Mw and Mn, resins and asphaltenes by oxidation and composition. On the other
 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838
Fig. 18. Relationships between PDI and rheological properties.
hand, a part of saturates and aromatics is volatilized. The former
two components are usually considered to be a lubricant and can
reduce the viscosity and improve the fluidity of bitumen. However,
the latter two components are usually considered to have higher
viscosity. Thus, as the aging increases, the increase of LMS and
decrease of MMS causes an increase in PDI, leading to the increase
in G*, S, and Nf, and the decrease in d and m-value. Above all,
according to the strong correlation between PDI and rheological
properties, the parameter PDI got by GPC may be feasible to
describe and predict the rheological properties of bitumen.
3.3.4. Relationship between indexes of FT-IR and GPC
Fig. 19 presents the relationship between the carbonyl index
and the polydispersity. The carbonyl index shows a good but not
perfect linear correlation with PDI. The correlation indicates that
the conversion of SMS to MMS and MMS to LMS are mainly caused
by oxidation, but there are other reasons at the same time. For
example, maybe a part of LMS is composed of multiple MMSs and
SMSs, and a part of MMS is composed of multiple SMSs. Besides,
parts of LMS may be decomposed into SMSs as aging goes on, which
has also been discussed in 3.3.3. According to the analysis, several
different reaction processes during aging are proposed, as shown in
Fig. 20.
According to the previous analysis, both the carbonyl index and
polydispersity have a strong correlation with the rheological prop-
erties of bitumen. The carbonyl index represents the degree of
6.0
5.5 PDI
5.0
4.5
PDI
4.0
3.5
PDI=2.20692Ic=o+3.01136
R2=0.83328
3.0
2.5
0.0 0.2 0.4 0.6 0.8 1.0
IC=O
Fig. 19. The relationship between the carbonyl index and polydispersity.
835
Fig. 20. Components shifting during aging.
components oxidation during the short-term aging. Moreover,
the polydispersity represents the degree of component migration
during the short-term aging, including composition, decomposi-
tion, volatilization, and absorption of oxygen. Therefore, it may
be feasible to use IC@O and PDI, obtained by chemical experiments,
to take the place of the traditional rheological test to predict the
rheological properties of bitumen, and the fitting results are listed
in Table 2.
4. Conclusions
Base on the rheological properties of bitumen, the time-
temperature equivalent effects of bitumen short-term aging has
been discussed in this study. Besides, the short-term aging mech-
anism of bitumen is also discussed by analyzing the indexes from
FT-IR and GPC, and the following conclusions can be drawn:
(1) As the aging situation shift from 163 °C/85 min to
191 °C/385 min, the G* at 64 °C, S at 12 °C and the Nf
(cmax = 2.5%) and Nf (cmax = 5%) increase, the d at 64 °C and
m-value decrease. Besides, according to the slopes of indexes
under different aging configurations, it can be concluded
that the fatigue resistance is most sensitive to aging, fol-
lowed by the low-temperature performance, and the high-
temperature performance is least susceptible to aging.
(2) According to the characteristics of rheological properties of
bitumen before and after the short-term aging, the time-
temperature equivalent conversion models of bitumen aging
base on the high/low-temperature performance are con-
structed, including the master curve at a reference tempera-
ture of 177 °C and shift factors at different temperatures.
(3) As the temperature increases, the growth rate of the carbonyl
index increases. The mass change of bitumen before and after
the short-term aging, caused by oxidation (increase the
836 W. Ye et al. / Construction and Building Materials 215 (2019) 823–838
Table 2
Formulas for predicting rheological properties.
Predicting formulas
2 3
G ¼ 22:065 þ 22:091IC¼O þ 52:006PDI  25:584PDI þ 3:5455PDI
d ¼ 30:778  12:100IC¼O þ 88:360PDI  21:102PDI2 þ 1:5236PDI3
S ¼ 34:709 þ 83:352IC¼O þ 93:784PDI  16:761PDI2 þ 1:4531PDI3
m ¼ 0:93567  0:049342IC¼O  0:31204PDI þ 0:055959PDI2  0:0036034PDI3
N f ðcmax ¼ 2:5%Þ ¼ 2:1149 107 þ 2:1857 106 IC¼O  1:7712 107 PDI þ 4:7754 106 PDI2  3:9849 105 PDI3
N f ðcmax ¼ 5%Þ ¼ 2:2418 105 þ 2:9599 104 IC¼O  1:8975 105 PDI þ 5:6073 104 PDI2  4:9478 103 PDI3
mass) and volatilization (decrease the mass), gradually
changes from a positive value to a negative value. It could
be concluded that both oxidation and volatilization are accel-
erated as the temperature increases, but the volatilization is
more sensitive to temperature than the oxidation.
(4) According to the results got by FT-IR and GPC, the oxidation
and the components’ migration (composition, decomposi-
tion, and volatilization) of bitumen would lead to an increase
in the proportion of large molecular size components, which
in turn lead to an increase in G*, S, and Nf, and a decrease in d
and m-value.
(5) Both the carbonyl index got by FT-IR, and the polydispersity
got by GPC have a strong correlation with rheological prop-
erties of bitumen. According to this, it may be feasible to
predict the rheological properties by carbonyl index and
polydispersity. Therefore, prediction models with strong
correlation coefficient are constructed.
Conflict of interest
No potential conflict of interest was reported by the authors.
Acknowledgments
This project was jointly supported by the National Natural
Science Foundation of China (Grant No. 51608043), the Youth
Top-notch Talent Support Program of Shaanxi Province, the Fok
Ying-Tong education foundation (Grant No. 161072), and the Fun-
damental Research Funds for the Central Universities (Grant No.
300102219317).
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.conbuildmat.2019.04.197.
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