Construction and Building Materials 220 (2019) 637–650

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Construction and Building Materials

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

Aging degradation of asphalt binder by narrow-band UV radiations with

a range of dominant wavelengths
Yuanyuan Li a,c,e, Shaopeng Wu a,⇑, Quantao Liu a, Ying Dai b, Chuangmin Li c,d,⇑, Hechuan Li a, Shuai Nie a,
Wei Song a
a
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China
b
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
c
School of Traffic and Transportation Engineering, Changsha University of Science and Technology, Changsha 410114, Hunan, China
d
Engineering Laboratory of Spatial Information Technology of Highway Geological Disaster Early Warning in Hunan Province, Changsha University of Science & Technology,
Changsha 410114, Hunan, China
e
Nottingham Transportation Engineering Centre, School of Civil Engineering, University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom

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

Aging degradations of five UV

radiations on asphalt were
investigated.

Chemical transitions of asphalt were
tested by FTIR and XPS after UV aging.

Macro-performance of asphalt was
also surveyed both before and after
UV aging.

Dominant wavelength of UV radiation
can obviously affect aging behavior of
asphalt.

UV–360 ages asphalt most seriously,
followed by UV–340, UV–320, UV–
300 and UV–380.

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

Article history: To investigate the aging degradations of dominant wavelength of UV radiation on asphalt binder, five
Received 14 March 2019 narrow-band UV radiations with different dominant wavelengths, namely 300, 320, 340, 360 and
Received in revised form 8 May 2019 380 nm, were used to age asphalt. After the UV aging, the aging degradations of the UV radiations on the
Accepted 3 June 2019
chemical compositions, physical properties, rheological properties and complex viscosities of asphalt binder
Available online 24 June 2019
were tested by Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS),
physical property test, and dynamic shear rheometer (DSR) respectively. The results show that all UV radi-
Keywords:
ations, with the dominant wavelengths from 300 nm to 380 nm, can cause the aging degradations on the
Modern testing techniques
Aging degradations
neat asphalt, UV aging can change the chemical compositions of asphalt, as well as the macro-
UV radiation parameters performance of asphalt, such as physical and rheological performance. While, the molecules of asphalt have
Asphalt Binder different susceptibilities to different wavelengths of UV radiations, different dominant wavelengths of UV
Dominant wavelength radiations have different aging degradations on asphalt, it is not that a UV radiation with shorter wavelength
Half-wavelength (higher photon energy) definitely produces more serious aging effect on asphalt. Making into comparison,
under the same aging condition, the asphalt binder aged by the UV – 360 has the highest aging degree, fol-
lowed with the asphalt binders aged by UV – 340, UV – 320, UV – 300 and UV – 380, respectively.
Ó 2019 Elsevier Ltd. All rights reserved.

⇑ Corresponding authors at: State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China (S. Wu); School of Traffic
and Transportation Engineering, Changsha University of Science and Technology, Changsha 410114, Hunan, China (C. Li).
E-mail addresses: liyuanyuan@whut.edu.cn (Y. Li), wusp@whut.edu.cn (S. Wu), liuqt@whut.edu.cn (Q. Liu), yingdai@whut.edu.cn (Y. Dai), lichuangmin@csust.edu.cn (C.
Li), lihc@whut.edu.cn (H. Li), nies1993@whut.edu.cn (S. Nie), songwei6695@whut.edu.cn (W. Song).

https://doi.org/10.1016/j.conbuildmat.2019.06.035
0950-0618/Ó 2019 Elsevier Ltd. All rights reserved.
638 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650
1. Introduction
For the excellent viscoelastic properties of asphalt [1], it is
widely used in road engineering, which satisfies the travel
demands of citizens, as well as promotes the development of the
economy. The physical and rheological performance of asphalt
has significant time and temperature dependence [2]. In order to
make sure that the asphalt pavement has good pavement perfor-
mance and long service life, the asphalt binder must maintain its
excellent viscoelastic properties during its service life. However,
during the life cycle of asphalt binder, it will be inevitably aged
by many factors, such as ultraviolet (UV) light [3,4], oxygen [5,6],
temperature [7], water [8,9] and vehicle loadings, etc. The aging
of asphalt in its life cycle includes thermo-oxidative aging and
UV aging, the thermo-oxidative aging mainly occurs during the
production, storage and construction of asphalt binder and its mix-
ture [10,11], while UV aging mainly occurs in the service phase of
asphalt pavement [12]. After aging, asphalt binder will be stiffer
and more brittle, as a result, the service life of asphalt pavement
will decrease significantly [13]. In last decades, the aging of asphalt
binder has gained more and more attention [14,15], the improve-
ment of the aging resistance of asphalt binder can not only
decrease the energy consumption, but also protect the environ-
ment and resources [16].
Compared to the thermo-oxidative aging of asphalt binder, there
is less work conducted on the UV aging of asphalt, especially for the
influence of UV radiation parameters on the UV aging effect of
asphalt binder. The UV radiation parameters includes dominant
wavelength, half-wavelength and irradiation intensity [17]. From
the quantum theory [18], the photon energy of UV radiation is differ-
ent with its wavelength, the shorter the wavelength of light, the
higher energy is the photon. In addition, from the first law of photo-
chemistry, different kinds of polymer structures have different sen-
sitivities to different optical wavelengths, if the wavelength is not
a sensitive wavelength for a macromolecular, the photodegradation
will be very light [19]. Therefore the wavelength of UV radiation
must match the sensitive wavelength of a polymer. These two theo-
ries have been made into consideration in the aging behavior of the
polymer field. Such as, Alexandre François-Heude [20,21] stated that
the carboxylic acids and esters have none or a weak photosensitivity
to the UV radiations with a wavelength of higher than 290 nm. Petri
Kärhä [22] investigated the aging degradations of radiation in the
wavelength range of 250–500 nm on sample, after being aged from
1 h to 8 h, the color changes were tested to characterize the aging
statuses of samples, the results indicated that the yellowness indices
of sample were different under the irradiation of radiation with dif-
ferent wavelengths, the aging behaviors of the samples have obvious
wavelength dependencies. Santos AL [23] investigated the biological
degradations of nine bacterial isolates under irradiations of UVA,
UVB and UVC, the results showed that the survival and activity of
these nine bacterial isolates had a obvious wavelength dependence.
Yousif E [19] studied the wavelength sensitivity of the poly (methyl
methacrylate) (PMMA) in the wavelength range of 250–1000 nm,
the results indicated that the radiation in the wavelength range of
260–320 nm could cause the main-chain scission of PMMA, but
the photodegradation phenomenon was not observed with the radi-
ation wavelength of longer than 340 nm. Asphalt is also a kind of
organic polymer material, UV radiations with different dominant
wavelengths may cause different aging degradations [24]. Mean-
while, whether a UV radiation with relative shorter wavelength
can cause more serious aging effect on an asphalt binder is still
not clear. So, it is of great significance to investigate the degradations
of wavelengths of UV radiations on the aging of an asphalt binder.
Because of the absorption effect of the stratosphere, the UV
radiation with the wavelength of lower than 290 nm can not reach
to the surface of earth [25], so it is more suitable and significant to
discuss the aging degradations of the UV radiations in the wave-
length range of 290–400 nm [19]. In the previous, researchers
always arbitrarily selected and applied only one dominant wave-
length to the UV aging simulation test of asphalt, such as 313 nm
[26], 340 nm [27,28], 365 nm [7]. In last year, our team used three
UV radiations with different dominant wavelengths to conduct the
UV aging test of asphalt, the results showed that UV radiation in
the range of 300–350 nm had the most serious aging effect on
asphalt, followed by UV radiations in the range of 260–300 nm
and 350–400 nm. But, due to the relative bigger half-wavelength
(20–25 nm) of them, the conclusions of which were more or less
fuzzy [17].
The research on the dominant wavelength effect on the UV
aging of asphalt can help us to know the sensitive wavelength of
asphalt, it can be used to guide the selection of anti aging additives
and improve the anti UV aging technologies of asphalt. In this
research, five kinds of UV radiations with the same half-
wavelength, same irradiation intensity and different dominant
wavelengths were used for the aging simulating test of asphalt bin-
der. The half-wavelengths of these five UV radiations are very
small (10 nm), which is able to make the wavelength range of UV
radiation to be divided more finely. The relative contents of chem-
ical functional groups of asphalt were detected by both Fourier
transform infrared spectroscopy (FTIR) and X-ray photoelectron
spectroscopy (XPS), the softening point test was conducted to test
the softening point of asphalt, the complex modulus, phase angle
and complex viscosity were studied by dynamic shear rheometer
(DSR), the results can be used to investigate the aging effects of
the dominant wavelengths of UV radiations on the chemical struc-
ture, physical and rheological performance changes of asphalt
before and after UV aging.
2. Materials and methods
2.1. Asphalt binder
A neat asphalt binder with 60/80 penetration grade was
selected to conduct the UV aging simulation test, which was
offered by Inner Mongolia Xindalu Asphalt CO., LTD (Inner Mongo-
lia, China). The technical information of asphalt binder is shown in
Table 1.
2.2. Experimental methods
2.2.1. UV aging simulation test in laboratory
The UV aging simulation test of asphalt binder was conducted
by a UV aging apparatus developed by ourselves, the UV radiation
generator of which can be equipped with different UV filters, by
which, this apparatus can produce five kinds of UV radiations with
different dominant wavelengths. The transmission ranges of UV
radiations of different filters are shown in Fig. 1.
In total five kinds of UV radiations were simulated in the labo-
ratory to conduct the UV aging test of asphalt binder, these five UV
radiations have the same half-wavelength of 10 nm, while have
different dominant wavelength ranges namely 300 nm (UV –
300), 320 nm (UV – 320), 340 nm (UV – 340), 360 nm (UV – 360)
and 380 nm (UV – 380). There is no coincident wavelength range
of these five UV radiations. The irradiation intensity of all UV radi-
ations was 7.0 w/m2. Eight levels of UV aging times, namely 1, 3, 6,
12, 24, 72, 144 and 216 h, were designated for the every UV radia-
tion. The thickness of asphalt sample for UV simulation test was
1.5 mm. The temperature of the chamber of UV aging apparatus
was 25 °C, while due to the thermal radiation of UV lamps, the
temperature of the surface of asphalt binders was about 50 °C.
 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650 639

Table 1
Technical information of asphalt binder.

Asphalt Technical information Units Results Requirements Methods

Virgin 25 °C penetration 0.1 mm 66.3 60–80 ASTM D5 [29]
Softening point °C 51.0 46 ASTM D36 [30]
60 °C dynamic viscosity Pa.s 302.500 180 ASTM D4402 [31]
10 °C ductility cm 165 15 ASTM D113 [32]
After TFOT Mass loss % 0.13 ±0.8 ASTM D2872 [33]
25 °C residual penetration ratio % 61 61 ASTM D5
10 °C ductility cm 66 6 ASTM D113
Softening point °C 52.5 – ASTM D36

100 100
290~310nm 310~330nm 330~350nm
90 90 P365L E365
350~370nm 370~390nm
80 80

Photoresponsivity (a.u.)
70 70
Transmittance (%)

60 60

50 50

40 40

30 30

20 20

10 10

0 0
280 290 300 310 320 330 340 350 360 370 380 390 400 240 260 280 300 320 340 360 380 400 420
Wavelength (nm) Wavelength (nm)

Fig. 1. Transmission ranges of UV radiations of different filters. Fig. 2. Spectral corresponding curves of the probes of UV irradiation meter.

The parameters of UV aging test of asphalt binder are concluded

of C element with O element. The etch depth was less than
and listed in Table 2.
5 nm. The XPS instrument (Thermo ESCALAB 250XI, Axis
The irradiation intensities of UV – 300, UV – 320 and UV – 340
Ultra DLD Kratos AXIS SUPRA, PHI-5000versaprobe) was
were detected by the P365L probe, and the E365 probe was used
used in this research, the energy step size was 1.00 eV, the
for the UV – 360 and UV – 380 nm. The spectral corresponding
number of energy steps was 1000 (0–1000 eV).
curves of both P365L and E365 probes are shown in Fig. 2.

2.2.2. Chemical analysis test 2.2.3. Softening point test

(1) Fourier transform infrared spectroscopy test
Fourier transform infrared spectroscopy (FTIR) instrument
was conducted to test the chemical functional groups of
asphalt before and after UV aging, respectively. The asphalt
films used for the FTIR test were prepared with solution
forming film method, the substrate was potassium bromide
window piece. The solvent was carbon disulfide. The sweep
time for every sample was 32 times, the sweep wavenumber
range of all samples was from 400 cm1 to 4000 cm1.
(2) X-ray photoelectron spectroscopy test
X-ray photoelectron spectroscopy (XPS) test is a highly sen-
sitive technique to analyze the element composition and
chemical state of the surface of solid substance [34]. On
one hand, the XPS was used to detect the exists and relative
contents of the C, H, O, N and S elements in asphalt binder,
meanwhile, it was also used to analyze the bonding states
The ring-and-ball softening points of asphalt binders before and
after UV aging were tested according to the criterion of ASTM D36
[30], the increments of softening points of asphalt binders after dif-
ferent UV aging statuses were calculated to investigate the physical
performance change of asphalt.
2.2.4. Rheological property test
A frequency sweep tests of asphalt binders before and after UV
aging was conducted by a dynamic shear rheometer (DSR), which
was done to test the rheological properties of asphalt, such as com-
plex modulus and phase angle. The diameter of rotor was 25 mm,
the gaps between the top and bottom plate was 1.0 mm for the
complex modulus and phase angle, while it was 0.05 mm for the
complex viscosity test. Before the rheological properties tests, all
of the samples were under the starting temperature for three min-
utes; during the test, the increasing rate of temperature was 3 °C/
min. The accuracy of temperature was ±0.01 °C. Meanwhile, the

Table 2
Parameters of UV aging test of asphalt binder.

UV radiation Dominant Wavelength Irradiation Aging time Temperature

wavelength (nm) range (nm) intensity (w/m2) (hours) (°C)
UV – 300 300 290 – 310 7.0 1, 3, 6, 12, 24, 72, 50
UV – 320 320 310 – 330 144 and 216
UV – 340 340 330 – 350
UV – 360 360 350 – 370
UV – 380 380 370 – 390
640 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650

complex viscosity of asphalt binder was also tested and recorded
by DSR.
3. Results and discussions
3.1. Chemical compositions analysis
The microscopic chemical composition of a substance is the root
of influencing the macroscopic physical and rheological properties
of which, the studies of the chemical compositions of asphalt bin-
der are good for understanding the mechanism of the performance
changes of asphalt during UV irradiation. In this chapter, both FTIR
and XPS instruments were conducted to study the chemical com-
positions and investigate the binding states of the elements of
asphalt binders at different aging degrees.
3.1.1. Relative contents of carbonyl and sulfoxide groups
During to the oxidation, asphalt can absorb the oxygen, the rel-
ative contents of oxygen-containing functional groups in asphalt
will increase, therefore, the relative contents of the oxygen-
containing functional groups can be used to characterize the aging
degree of asphalt, such as the carbonyl and sulfoxide groups [35].
The carbonyl group index (CGI) and sulfoxide group index (SGI)
were calculated according to the Eqs. (1) and (2), they express
the relative ratios of the areas of absorption bands of carbonyl
and sulfoxide groups to the total area of all the absorption bands,
respectively.
S1700 cm1
CGI ¼ ð1Þ
S2000 600 cm1
S1030 cm1
SGI ¼ ð2Þ
S2000 600 cm1
where S1700 cm1 is the area of the absorption band of carbonyl group
(1700 cm1), S1030cm1 is the area of the absorption band of sulfoxide
group (1031 cm1), S2000 600 cm1 is the areas of all absorption bands
in the wavenumber range of 2000–600 cm1.
The results of CGI and SGI of asphalt before and after aging are
shown in Fig. 3 and Fig. 4 respectively. It can be found from the
Fig. 3, compared with the CGI value of virginal asphalt binder,

0.0038
Aged by UV 300 Aged by UV 320
0.0036
Aged by UV 340 Aged by UV 360
0.0034
Aged by UV 380
0.0032
CGI values

0.0030

0.0028

0.0026

0.0024

0.0022

0.0020
0 20 40 60 80 100 120 140 160 180 200 220
Aging time (hour)

Fig. 3. CGI values of asphalt binder aged by different wavelengths of UV radiations.

0.0390

0.0360

0.0330
SGI values

0.0300

0.0270

0.0240 Aged by UV 300 Aged by UV 320

Aged by UV 340 Aged by UV 360

0.0210
Aged by UV 380
0.0180
0 20 40 60 80 100 120 140 160 180 200 220
Aging time (hour)

Fig. 4. SGI values of asphalt binder aged by different wavelengths of UV radiations.

 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650
the CGI values of asphalt binders increase after being aged by UV
radiations with different wavelengths, and the increments of CGI
values are more obvious with increasing aging times. For instance,
the CGI values of asphalt binder after 1, 3, 6, 12, 24, 72, 144 and
216 h of UV aging by the UV radiation with wavelength of
360 nm increase by 10.5%, 16.0%, 18.4%, 24.0%, 34.3%, 44.0%,
48.0% and 62.0%, respectively. From Fig. 4, the SGI values of asphalt
binders also increase after the UV aging, with the increase of aging
time, the SGI values increase more obviously. In detail, the SGI val-
ues of asphalt binder after 1, 3, 6, 12, 24, 72, 144 and 216 h of UV
aging by the UV radiation with wavelength of 360 nm increase by
1.7%, 7.9%, 18.1%, 27.4%, 36.5%, 45.8%, 55.0% and 59.9%, respec-
tively. In the first 24 h of UV irradiations, the CGI and SGI values
increase rapidly, while, the increasing rates of CGI and SGI values
will slow down when the aging times are longer than 24 h.
Meanwhile, with the irradiations of UV radiations with different
wavelengths, the increments of CGI and SGI values are different.
When the aging time is 24 h, the CGI value of asphalt binder aged
by UV – 360 is 5.5%, 8.5%, 15.0% and 23.1% higher than that of UV –
340, UV – 320, UV – 300 and UV – 380 respectively, the SGI value of
asphalt binder aged by UV – 360 is 6.3%,9.7%, 28.0% and 43.2%
higher than that of UV – 340, UV – 320, UV – 300 and UV – 380
respectively; while after 216 h of UV irradiation, the CGI value of
asphalt binder aged by UV – 360 is 4.0%, 8.4%, 11.1% and 19.2%
higher than that of UV – 340, UV – 320, UV – 300 and UV – 380
respectively, the SGI value of asphalt binder aged by UV – 360 is
10.3%, 15.4%, 22.8% and 39.6% higher than that of UV – 340, UV –
320, UV – 300 and UV – 380 respectively. Therefore, the UV radia-
tion with the dominant wavelength of 360 nm has the most signif-
icant aging effect, followed by the UV – 340, UV – 320, UV – 300
and UV – 380. The increases of the relative contents of carbonyl
groups and sulfoxide groups can be thought to be the increase of
relative content of the oxygen element, it is caused by the absorp-
tion of oxygen element during the UV irradiation of asphalt. The
Fig. 5. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder before aging.
641
increasing contents of oxygen-containing polar functional groups
will cause to generate more complex side branched chains on
asphalt molecules. On the one hand, for the permanent dipoles
between the polar oxygen containing functional groups, the fric-
tion resistance between asphalt molecules increases, which may
lead to the increase effect on the viscosity of asphalt binder. In
addition, as the more complex side branched chain structure of
asphalt can hinder the internal rotation of the asphalt molecules
chain, result in the increase of the modulus of which. All these
effects make asphalt binder tend to be more brittle and harder.
3.1.2. Binding states analysis
The XPS test was performed on the asphalt binders before aging
and after 216 h of UV irradiation respectively, which can detect the
binding states of the elements in asphalt binder. The correction
values for charge corrections of all elements were determined
according to the C 1s spectrum at 284.5 eV. The XPS spectrums
of different elements of asphalt binders aged by different UV radi-
ations are shown in Figs. 5–10.
From Fig. 5a, the C 1s peak of virginal asphalt binder is very
symmetric, the spectrum of which is a horizontal line with no peak
at the binding energy of higher than 286 eV. It is deconvoluted in
two peaks, the main one at the 284.5 eV is the CAC or CAH bonds,
it accounts for 98.6 At.%; the other one at the 286.2 eV attributes to
the bonds between carbon and oxygen (such as the CAO, C@O and
O@CAO), it accounts for only 1.4 At.%. That means the C atom in
the virginal asphalt is mostly in the form of CAC or CAH bond,
there is very low content of O atom in the virginal asphalt, indict-
ing almost no aging in the virginal asphalt. Due to the very low
content of C atom bonds with O atom, it is difficult to distinguish
the state of carbon binding to oxygen in the C 1S spectrum, so
the O 1S spectrum is also analyzed. In the Fig. 5b, the O 1S spec-
trum is divided into three peaks, the binding energy at 531.4 eV
belongs to the OAC bond, the binding energy at 532.1 eV belongs
642 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650

Fig. 6. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder aged by UV 300 nm.

Fig. 7. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder aged by UV 320 nm.
 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650 643

Fig. 8. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder aged by UV 340 nm.

Fig. 9. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder aged by UV 360 nm.

to the O@C bond, and the binding energy at 533.7 eV is assigned to around the 400 eV can be attributed to the N bonds, it is divided
the O@CAO bond, the relative content of them are 46.3 At.%, into two peaks, which indicate the two binding statuses of N atom,
39.9 At.% and 13.8 At.% respectively. In Fig. 5c, the main peak the first is the Pyridinic-N peak at the binding energy of 398.9 eV,
644 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650

Fig. 10. C 1s (a), O 1s (b), N 1s (c) and S 2p (d) XPS spectrums of asphalt binder aged by UV 380 nm.

the second is the Pyrrolic-N peak at the binding energy of 400.4 eV,
the ratios of these two binding statuses are 51.6 At.% and 48.4 At.%
respectively. In Fig. 6d, the two peaks at binding energies of
143.4 eV and 164.5 eV belong to the sulfoxide (S@O) and sulfone
(O@S@O) bonds respectively [36], they account for 86.8 At.% and
13.2 At.% in the whole content of S atoms.
For the C 1s XPS spectrums, after being aged by UV – 300, UV –
320, UV – 340, UV – 360 and UV – 380, the ratios of C atoms bond
with O increase from 1.4 At.% to 3.5 At.%, 3.7 At.%, 12.4 At.%, 17.0
At.% and 1.5 At.% respectively, meanwhile the ratios of C bonds
with C decrease from 98.6 At.% to 96.5 At.%, 96.3 At.%, 87.6 At.%,
83.0 At.% and 98.5 At.% respectively, which shows that there are
higher ratios of C atoms bind with O after UV aging. For the O 1s
XPS spectrums, the ratios of O-C bonds decrease significantly
under UV expose, while the ratios of O@C and O@CAO bonds
increase obviously. In detail, the ratios of O@C and O@CAO bonds
of asphalt binder aged by UV – 360 have the highest increment, fol-
lowed by the asphalt binders aged by UV – 340, UV – 320, UV – 300
and UV – 380. Therefore, the contents O atoms will increase after
UV irradiation. For the N 1s XPS spectrums, because of the relative
lower content of N atom in asphalt binder (only about 1.0 At.%), the
XPS results of which may have heavy fluctuations, so there is no
specific trends were correlated with the ratios of N atoms in differ-
ent binding states. For the S 2p XPS spectrums, after aging, the
O@S@O bond peak tend to be more obvious, the ratio of which
increases significantly, especially the asphalt binder aged by UV
– 360 has the highest increment, that means the S atom can bond
with more O atoms. The results of XPS analysis of asphalt binder
show that there will be more O atoms exist in the aged asphalt bin-
der, which is agree with the result of FTIR analysis, the contents of
the oxygen-containing functional group of the aged asphalt is
higher than that of virginal asphalt binder.
3.2. Physical property analysis
The physical property of asphalt was characterized basing on
the softening point of which, the softening point test of asphalt
binder was conducted before and after different statuses of UV
aging respectively. The results of softening points of asphalt bin-
ders after aging are shown in Table 3. From Table 3, the softening
points of all asphalt binder after exposing to the UV radiation with
different dominant wavelengths tend to increase, meanwhile the
increments of softening points increase with increasing aging
times, which shows a stiffness effect of UV radiation on the asphalt
binders.
The softening point increments of asphalt binders during UV
aging were calculated according to the equation (3), the results
are going to be used to quantitatively evaluate the changes of soft-

Table 3
Softening points of asphalt binders before and after aging.

Dominant wavelength (nm) Softening points (°C) of asphalt binders after UV irradiation for the following times (h)
0 1 3 6 12 24 72 144 216
300 51.0 52.2 53.3 53.9 54.0 54.4 54.5 55.3 56.0
320 51.0 52.8 53.1 53.3 54.1 54.9 55.3 56.0 56.5
340 51.0 53.2 53.4 54.7 55.1 55.7 55.9 56.8 57.6
360 51.0 53.8 54.4 55.0 55.5 56.3 56.8 57.4 58.7
380 51.0 52.0 52.6 53.0 53.6 53.8 54.2 54.8 55.2
 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650 645

9 2.5 °C higher than that of aged by the UV radiation with the dom-
300 nm 320 nm 340 nm
inant wavelength of 340 nm, 320 nm, 300 nm and 380 nm, respec-
8
360 nm 380 nm tively; while after 216 h of UV irradiation, that are 1.1 °C, 2.2 °C,
7 2.7 °C and 3.5 °C, respectively. Therefore, the UV radiation with
Softening point incrments (°C)

the dominant wavelength of 360 nm has the most significant aging

6
effect, followed by the UV – 340, UV – 320, UV – 300 and UV – 380.
5

4
3.3. Rheological performance before and after aging

3 For the viscoelastic performance of asphalt, both the tempera-

2
ture and loading frequency can obviously affect the complex mod-
ulus (G*) and phase angle (d) of asphalt, the mechanical response of
1 which follows the time-temperature equivalence principle [37,38].
0
That means, when under different temperature conditions, the
0 20 40 60 80 100 120 140 160 180 200 220 same mechanical response can be obtained by using an appropri-
Aging time (hour) ate loading frequency; similarly, under the condition of different
loading frequencies, the same mechanical response can also be
Fig. 11. Softening point increments (SPI) of asphalt binders during UV aging.
obtained by loading for an appropriate time [39]. In this research,
the frequency sweep test was conducted at temperatures of 40, 46,
52, 58, 64, 70, 76 and 82 °C respectively, the sweep frequency for
ening points of asphalt during UV aging. The results are shown in
every temperature was from 0.1 Hz to 100 Hz. The time-
Fig. 11.
temperature equivalence performance of asphalt can be character-
SPI ¼ SPaged  SPv irgin ð3Þ ized with WLF equation [40], shown as Eq. (4).

log½aðT Þ ¼ logf r  logf ð4Þ

where SPI expresses the softening point increments of asphalt bin-
ders after UV aging, °C; SPvirgin expresses the softening point of where log(a(T)) is the shift factor; fr expresses the reduced fre-
asphalt binder before UV aging, °C; SPvirgin expresses the softening quency, Hz; f is the actual frequency of test, Hz; T is the experimen-
point of asphalt binder after UV aging, °C. tal temperature, °C.
A positive value of SPI can be thought to be that the softening The master curves of complex moduli and phase angles of
points of asphalt will increase after UV aging, the higher the value asphalt binders aged by different UV radiations are shown from
of SPI indicates that the aging effect of asphalt is more obvious. Figs. 12 to 16. From Figs. 12 to 16, the complex moduli of asphalt
From Fig. 11, the SPI values of all asphalt binders after UV irradia- binders increase with the increase of reduced frequency, and the
tion show an increasing tendency with increasing aging times, phase angles of asphalt binders decrease, which conforms the sig-
which express an increasing aging degrade of asphalt binders. nificant dependence of the rheological performance of asphalt on
Comparing the SPI values of asphalt binders under the irradiations the reduced frequency (or temperature). It can be also observed
of UV radiations with different dominant wavelengths, after same that a consistent and obvious tendency can be observed, after the
aging times, the UV radiation with the dominant wavelength of aging of UV radiations, the complex moduli of asphalt binders
360 nm has highest SPI values. For instance, after 24 h of UV irra- increase, meanwhile, the phase angles of them decrease. At low
diation, the SPI values of asphalt aged by the UV radiation with frequency region, the phase angle differences of asphalt binders
the dominant wavelength of 360 nm are 0.6 °C, 1.4 °C, 1.9 °C and after different aging times is relatively small; while with the

1.E+07 95

90
1.E+06
85

1.E+05 80
Complex modulus (Pa)

Phase angle (°)

75
1.E+04
70
1.E+03
65

1.E+02 60
G*-vrigin G*-1 hour G*-3 hours
G*-6 hours G*-12 hours G*-24 hours 55
1.E+01 G*-72 hours G*-144 hours G*-216hours
δ-vrigin δ-1 hour δ-3 hours 50
δ-6 hours δ-12 hours δ-24 hours
δ-72 hours δ-144 hours δ-216 hours
1.E+00 45
0.0001 0.001 0.01 0.1 1 10 100
Reduced frequency (Hz)

Fig. 12. Master curves of complex modulus and phase angle of asphalt after aging of UV – 300.
646 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650

1.E+07 95

90
1.E+06
85

1.E+05 80
Complex modulus (Pa)

Phase angle (°)

75
1.E+04
70
1.E+03
65

1.E+02 60

G*-vrigin G*-1 hour G*-3 hours 55

1.E+01 G*-6 hours G*-12 hours G*-24 hours
G*-72 hours G*-144 hours G*-216 hours
δ-vrigin δ-1 hour δ-3 hours 50
δ-6 hours δ-12 hours δ-24 hours
1.E+00 45
0.0001 0.001 0.01 0.1 1 10 100
Reduced frequency (Hz)

Fig. 13. Master curves of complex modulus and phase angle of asphalt after aging of UV – 320.

1.E+07 95

90
1.E+06
85

1.E+05 80
Complex modulus (Pa)

Phase angle (°)

75
1.E+04
70
1.E+03
65

1.E+02 60
G*-vrigin G*-1 hour G*-3 hours
G*-6 hours G*-12 hours G*-24 hours 55
1.E+01 G*-72 hours G*-144 hours G*-216hours
δ-vrigin δ-1 hour δ-3 hours 50
δ-6 hours δ-12 hours δ-24 hours
δ-72 hours δ-144 hours δ-216 hours
1.E+00 45
0.0001 0.001 0.01 0.1 1 10 100
Reduced frequency (Hz)

Fig. 14. Master curves of complex modulus and phase angle of asphalt after aging of UV – 340.

increase of loading frequency, the differences become more signif-
icant. The increasing tendency of complex moduli indicates the
ability of asphalt to resist deformation under the repeated shear
loading is enhanced, and the decreasing tendency of phase angles
shows the ratio of elastic modulus (or storage modulus) of the
complex modulus [41] is increased after UV aging. The reason is
that, during the UV irradiation, on the one hand, the molecules of
asphalt can be oxidized and molecules weight are increased for
the oxidative condensation; in addition, some light components
in asphalt can volatilize, the light components’ ratios in asphalt
decrease, while the weight components’ ratios in asphalt increase,
the equilibrium between different components of asphalt is
destroyed. The changes of chemical compositions of asphalt cause
the deteriorations on the physical and rheological performance of
which. Making into comparison, under a same experimental condi-
tion (temperature, aging time and irradiation intensity), the
asphalt binder aged by the UV radiation with the dominant wave-
length of 360 nm has the highest aging degree, followed by the UV
radiations with the wavelengths of 340 nm, 320 nm, 300 nm and
380 nm.
For instance, after different times of UV radiations, the complex
moduli aging indices (CMAI) of asphalt binders at 1.0 Hz and 40 °C
is shown in Fig. 17. The CMAI was defined as the Eq. (5).
CMaged  CM v irgin
CMAI ¼  100 ð5Þ
CM v irgin
 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650 647

1.E+07 95

1.E+06
85

Complex modulus (Pa) 1.E+05

Phase angle (°)

75
1.E+04

1.E+03
65

1.E+02
G*-vrigin G*-1 hour G*-3 hours
G*-6 hours G*-12 hours G*-24 hours 55
1.E+01 G*-72 hours G*-144 hours G*-216 hours
δ-vrigin δ-1 hour δ-3 hours
δ-6 hours δ-12 hours δ-24 hours
δ-72 hours δ-144 hours δ-216 hours
1.E+00 45
0.0001 0.001 0.01 0.1 1 10 100
Reduced frequency (Hz)

Fig. 15. Master curves of complex modulus and phase angle of asphalt after aging of UV – 360.

1.E+07 95

90
1.E+06
85

1.E+05 80
Complex modulus (Pa)

Phase angle (°)

75
1.E+04
70
1.E+03
65

1.E+02 G*-vrigin G*-1 hour G*-3 hours 60

G*-6 hours G*-12 hours G*-24 hours
G*-72 hours G*-144 hours G*-216hours 55
1.E+01 δ-vrigin δ-1 hour δ-3 hours
δ-6 hours δ-12 hours δ-24 hours 50
δ-72 hours δ-144 hours δ-216 hours
1.E+00 45
0.0001 0.001 0.01 0.1 1 10 100
Reduced frequency (Hz)

Fig. 16. Master curves of complex modulus and phase angle of asphalt after aging of UV – 380.

where CMAI is the complex moduli aging indices of asphalt binders,
%; CMaged and CMvirgin are complex moduli of asphalt binders before
and after UV aging respectively, Pa.
The CMAI express the ratios of increments of complex moduli
during UV irradiation, the higher the values of CMAI are, the more
serious is the aging effect. From Fig. 17, all the CMAI values of
asphalt binders increase with the increase of aging time. After a
same aging time, the CMAI value of asphalt binder under the irra-
diation of UV radiation with 380 nm wavelength is the highest. In
detail, after 24 h of UV irradiation, the CMAI value of asphalt binder
under the irradiation of UV radiation with 360 nm wavelength is
39.7%, 54.1%, 61.8% and 201.1% higher than that of 340 nm,
320 nm, 300 nm and 380 nm respectively; while after 216 h of
UV irradiation, that is 17.4%, 27.2%, 32.6% and 427.5% respectively.
Therefore, different wavelength of UV radiations have different
aging degradations on asphalt binder, the order of the aging effect
on the asphalt binder is UV – 360 > UV – 340 > UV – 320 > UV –
300 > UV – 380.
3.4. Complex viscosity of asphalt before and after aging
In general, the viscosity of an asphalt binder always increases
gradually with increasing times of UV irradiation [42,43]. In this
research, the complex viscosities of asphalt binders after the aging
of different UV radiations were also tested by the DSR. The param-
eter of complex viscosity aging index (CVAI) is defined as Eq. (6) to
characterize the amplification of the complex viscosities of asphalt
binders.
648 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650

220

200 UV - 300 UV - 320 UV - 340 UV - 360 UV - 380

180
Complex moduls aging index (%) 160

140

120

100

80

60

40

20

0
1 3 6 12 24 72 144 216
Aging time (hour)

Fig. 17. CMAI of asphalt binders aged by different UV radiations.

Table 4 A power function model, CVAI = atb (t is the aging times, h; a

Parameters of CVAI models under the irradiation of different UV radiations. and b are regression parameters), was used to investigated the
relationship between the values of CVAI of asphalt binders after
Dominant wavelength (nm) a b R2
UV irradiation under different UV radiations and aging times. The
300 17.250 0.4332 0.9018
parameters of the power function model are shown in Table 4. It
320 8.7462 0.5257 0.9584
340 6.1570 0.5714 0.9804 can be observed from Table 4, the correlation coefficients (R2) of
360 4.1478 0.6274 0.9913 asphalt binders after all UV irradiations are higher than 0.90, which
380 4.1697 0.4451 0.9327 means that there is a strong exponential relationship between the
values of CVAI of asphalt binders after UV irradiation under differ-
ent UV radiations and aging times. The different a and b values
CVaged  CVv rgin indicate the different aging behaviors of asphalt binders under
CVAIt ¼  100% ð6Þ
CVv rgin the irradiations of different UV radiations.
The values of CVAI and the power function models of asphalt
where CVAIt is the complex viscosity aging indices of asphalt bin- binders after UV aging are shown in Fig. 18. From Fig. 18, the CVAI
ders after different times of UV aging, %; CVvirgin and CVaged are values of asphalt binder increase with increasing UV irradiation
the complex viscosity asphalt binders before and after different time, the longer the aging time, the more serious is aging degree
times of UV aging respectively, Pa. of asphalt binder. After 24 h of aging, the CVAI value of asphalt bin-

Fig. 18. VAI values of asphalt binders aged by different UV radiations.

 Y. Li et al. / Construction and Building Materials 220 (2019) 637–650
der aged by UV – 360 is 65.7%, 117.7%, 162.1% and 201.1% higher
than that of UV – 340, UV – 320, UV – 300 and UV – 380 respec-
tively; after 216 h of UV irradiation, the CVAI value of asphalt bin-
der aged by UV – 360 is 21.1%, 37.3%, 48.3% and 427.4% higher than
that of UV – 340, UV – 320, UV – 300 and UV – 380 respectively.
Therefore, the molecules of asphalt binder have obvious depen-
dence on the wavelength of UV radiations, the most sensitive
wavelength of asphalt binders in the wavelength range of 290–
390 nm is 360 nm, then is the 340 nm, 320 nm, 300 nm and
380 nm. The change tendency is coincide well with the above
experiments. The molecules of asphalt binder have different sus-
ceptibilities to UV radiations with different wavelengths, different
dominant wavelengths of UV radiations have different aging degra-
dations on asphalt, it is not that a UV radiation with shorter wave-
length (higher photon energy) must be able to produce more
serious aging effect on an asphalt binder. Making into comparison,
under the same aging condition, the asphalt binder aged by the UV
– 360 has the highest aging degree, followed with the asphalt bin-
ders aged by UV – 340, UV – 320, UV – 300 and UV – 380,
respectively.
4. Conclusions
In this research, to investigate the effect of dominant wave-
length of UV radiation on the aging of an asphalt binder, five kinds
of UV radiations were used for the aging simulating test of neat
asphalt. After different UV aging degrees, the chemical composi-
tions, complex viscosities, physical and rheological performance
of asphalt were investigated. The following conclusions can be
obtained.
(1) All the UV radiations, with the dominant wavelengths of
300 nm, 320 nm, 340 nm, 360 nm and 380 nm, can cause
the aging effect on the neat asphalt binder;
(2) XPS and FTIR results show that the UV radiations can signif-
icantly change the chemical compositions of asphalt, there
will be more O atoms exist in the aged asphalt binder, the
contents of the oxygen-containing functional group of the
aged asphalt is higher than that of virginal asphalt binder;
in addition, the physical and rheological performance test
show that the macro-performance of asphalt binder will also
changed obviously during UV aging;
(3) UV radiations with different dominant wavelengths have
different aging degradations on asphalt binders, therefore,
the molecules of asphalt binder have different susceptibili-
ties to UV radiations with different wavelengths. Meanwhile,
it is not that a UV radiation with shorter wavelength (higher
photon energy) must be able to produce more serious aging
effect on an asphalt binder;
(4) Under the same aging condition, the asphalt binder aged by
the UV – 360 has the highest aging degree, followed with the
asphalt binders aged by UV – 340, UV – 320, UV – 300 and
UV – 380, respectively.
Funding
The authors acknowledge the financial supported by the
National Key Research and Development Program of China (No.
2017YFE0111600), the Natural Science Foundation of China (No.
51778515), and the Open Fund of Engineering Laboratory of Spatial
Information Technology of Highway Geological Disaster Early
Warning in Hunan Province (Changsha University of Science &
Technology) (No. kfj180601).
649
Author contributions
Shaopeng Wu, Ying Dai, and Yuanyuan Li conceived and
designed the experiments. Yuanyuan Li, Hechuan Li, Shuai Nie
and Wei Song performed the experiments. Chuangmin Li and Yua-
nyuan Li analyzed the data. Ying Dai and Quantao Liu contributed
reagents/materials/analysis tools. Quantao Liu and Yuanyuan Li
wrote the paper. Shaopeng Wu and Quantao Liu reviewed the
paper.
Declaration of Competing Interest
The authors declare no conflict of interest.
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