Available online at SciVerse ScienceDirect

J. Mater. Sci. Technol., 2013, 29(7), 589e594

Nanomaterials Applied in Asphalt Modication: A Review

Changqing Fang1)*, Ruien Yu1,2), Shaolong Liu1), Yan Li2)*
1) College of Printing and Packing Engineering, Xian University of Technology, Xian 710048, China
2) School of Mechanical and Precision Instrument Engineering, Xian University of Technology, Xian 710048, China
[Manuscript received December 28, 2012, in revised form February 28, 2013, Available online 8 April 2013]

Nanotechnology has been gradually penetrated into the field of asphalt modification. Seemingly magic effects of
nanomaterials have now been brought to improve the performance of asphalt. To demonstrate many of the
prospective applications, researchers have conducted a series of positive and effective efforts dealing with
the preparation of modified asphalt to demonstrate the mechanism of modification and the resultant
improvement in performance. In this review, various nanomaterials used in asphalt modification are initially
presented, followed by the methods employed to modify the asphalt with these materials and finally the
effects of nanomaterials on the performance of base asphalt are presented and the modification mechanisms
are discussed. Based on the current research results, the influence of preparation process parameters on the
compatibility of every phase in the modified asphalt and the stability of the modified asphalt system are
described. Finally, the development trend of the topic field is projected.

KEY WORDS: Nanomaterials; Asphalt; Modication; Composites; Properties

1. Introduction nanotechnology has gradually been incorporated into the eld of

Nanomaterials are of morphological features on the nanoscale,
and especially have special properties stemming from their
nanoscale dimensions[1]. Since polyamide 6/clay nanocomposite
with excellent performance was prepared by Toyota research
center, the polymer grade nanocomposites have attracted
considerable interest in both academia and industry due to their
unique mechanical, thermal, barrier, optical, electrical, and mag-
netic properties[2,3]. Materials science and technology research is
focused on materials at macro to micro or nanoscale. With various
material states, liquid, semisolid or solid, asphalt is a black or dark
complex mixture containing hydrocarbons of varying molecular
weight and nonmetallic derivatives. Asphalt is usually employed
as an organic binding material for waterproong, moisture resis-
tance and corrosion protection[2,4]. Modication of base asphalt is
required to improve the materials performance (e.g. adhesion,
temperature sensitivity, friction properties, oxidation resistance,
aging resistance and durability). There are many kinds of asphalt
modiers, including various resins, rubbers, polymers, sulfur,
metal complexes, bers and chemical agents[4]. In recent years,
modied asphalt with various kinds of nanomaterials being used
to modify asphalt[1]. Fig. 1 illustrates the length scales evolution of
an asphalt concrete material, from macro scale to meso, micro,
nano and quantum scales[5]. The microstructure is the sole
determinant of macro properties, thus nano-modied asphalt of-
fers a signicant improvement over the fundamental material
properties, which is superior to other asphalt modication
methods. In August 2006, a National Science Foundation (NSF)
workshop entitled Nanomodication of Cementitious Materials
was held in the USA, which focused on using nanotechnology for
improvement of asphalt concrete. One of the main conclusions of
this workshop was that nanoscience and nanotechnology could
lead to improvements in asphalt pavement technology. In this
workshop the eld of asphalt nano-material science was
established[5,6]. In this review, various preparation methods of
nano-modied asphalts are analyzed, and the inuence of nano-
materials on the base asphalts properties and the mechanisms are
summarized.
2. Various Nanomaterials Used in Asphalt Modication

Various polymer modiers impart different inherent charac-

* Corresponding author. Prof., Ph.D.; Tel.: 86 29 82312038; Fax: 86
29 83212512; E-mail addresses: fcqxaut@163.com (C. Fang), jxxy-ly@
xaut.edu.cn (Y. Li).
1005-0302/$ e see front matter Copyright 2013, The editorial ofce of
Journal of Materials Science & Technology. Published by Elsevier
Limited. All rights reserved.
http://dx.doi.org/10.1016/j.jmst.2013.04.008
teristics to composites. Through research and development,
several good asphalt modiers such as: polyethylene (PE),
ethylene vinyl acetate (EVA), rubber and styrene butadiene
styrene (SBS) block copolymer, have been identied. The
lightweight, porous SBS has both the elastic properties of a
rubber and the thermoplastic properties of a resin, which allows
for a wide range of applications. However, some resins (such as
590 C. Fang et al.: J. Mater. Sci. Technol., 2013, 29(7), 589e594
Fig. 1 Illustration of the evolution of different asphalt dimensions[6].
PE) are relatively inexpensive, obtainable from recycled plastics
and can be mixed directly into base asphalt. Therefore, many
researchers are still committed to polymer modied asphalt,
working toward avoiding the drawbacks of this material in order
to prolong its use in pavement engineering[2]. One of the major
shortcomings of pure polymer modiers is that most of the
polymers are thermodynamically incompatible with asphalt due
to the large differences of density, polarity, molecular weight and
solubility between the polymer and the asphalt. This can result in
delamination of the composite during thermal storage, which is
not readily apparent and adversely affects the material when it is
used in construction.
In China, Yu and Wu et al. in Wuhan University of Technol-
ogy[7e14] reported the modication of base asphalt and SBS
modied asphalt using nanolayered silicate. Nano-SiO2, TiO2 and
CaCO3 were combined with SBS to modify base asphalt by Ye and
Chen[15], and Ma et al.[16e18] in Changan University. In addition,
researchers in Shandong Jiaotong University[1,2,19,20], Yangzhou
University[21e23], Chongqing Jiaotong University[24e26], Chang-
sha University of Science and Technology[27,28] and Hunan Uni-
versity[29] have also reported the aforementioned inorganic
nanomaterials as well as nanomaterials like Fe3O4 or ZnO to
directly modify base asphalt or combined with SBS or styrene
butadiene rubber (SBR) to modify base asphalt. Ouyang et al.[30e32]
in Shanghai Jiao Tong University have investigated the thermal
storage of asphalt modied with low density polyethylene (LDPE)
and silicate clay. In addition, the inuence of Kaolin clay on the
properties of SBS modied asphalt and styrene ethylene butadiene
styrene (SEBS) linear triblock copolymer modied asphalt was also
reported. It was found that the aging resistance, rheological and
thermal storage properties of asphalt modied with nanomaterials
are enhanced, thus the service life of the asphalt pavement is
prolonged[33].
Galooyak et al.[34], and Jahromi and Khodaii[35] discussed the
inuence of montmorillonite (MMT) and other nanoclays on the
rheological properties of SBS-modied and base asphalt. Goh
et al.[36] prepared nanoclay and carbon-microber-modied
asphalt and reported the mechanical properties and water resis-
tance of the asphalt mixtures. Kebritchi et al.[37] initially coated
polymers on the surface of CaCO3 and then this polymer/particle
composite was employed as an asphalt modier and the resultant
rheological properties of the modied asphalt were reported.
Sureshkumar et al.[38] prepared an EVA/nano-layered material
composite asphalt binder and investigated the properties and
mechanism of the bitumen/polymer/nano triple system. Zare-
Shahabadi et al.[39] used bentonite clay (BT) and synthesized
organic bentonite (OBT) to modify base asphalt and analyzed the
effect of modiers on the rheological properties of the modied
asphalt. Polacco et al.[40,41] also studied the inuence of layered
nanomaterials on SBS modied asphalt, and exhaustively
analyzed the effects of the polymer and the nanomaterial on the
base asphalt and speculated on the mechanisms involved in the
resultant viscoelastic and rheological properties.
Due to complex preparation methods, nanoscale organic ma-
terials are difcult to obtain by using conventional techniques,
thus commonly used polymer modiers are not readily available
as nano asphalt modication additives. However, metal oxide
nanomaterials can be prepared in a convenient way so they are
more likely to be used as base asphalt additives, therefore,
forming a promising method for modifying asphalt. However,
the high cost and characteristics of metal oxide nanomaterials
have limited their appeal in asphalt modication in both research
and application[1]. Theoretically, the vast majority of inorganic
metal oxide materials can be prepared as nanoscale materials
which can then be used to form nanocomposites with base
asphalt. But the key to success in accomplishing this is to nd a
dispersing surfactant that is compatible with both the nano ad-
ditives and the base asphalt. As previously reported, certain
inorganic metal oxide nanomaterials have occupied a dominate
position in asphalt modication, among which the most widely
used has been the layered clay nanomaterials, primarily MMT,
organic montmorillonite (OMMT). Base asphalt nanosized
modication technology is currently a popular area of research in
the eld of materials research and applications and also a driving
force in economic growth of transportation development.
3. Preparation and Processing of Modied Asphalt
Generally speaking, there are currently two main methods
used for asphalt modication[4]. One is high-speed shearing, the
most widely used and mature technology, by which the polymer
modier can be evenly dispersed in asphalt using a shearing
device. The second technique is termed mother liquor melting
and entails dissolving the polymer modier in an organic solvent
to prepare a highly concentrated polymer solution (mother li-
quor), followed by incorporation of the mother liquor into the
asphalt by mixing. The nal step involves heating the mixture to
distill and recover the solvent under high temperature conditions.
The compatibility between the modier and asphalt is the key to
improving asphalt modication effects. The compatibility de-
pends on the components of base asphalt, as well as the polarity,
particle size and molecular structure of the polymer modier and
the interfacial interaction between the asphalt and polymer
modier. The type of the modifying agent, preparation temper-
ature and modication process also inuence the performance of
modied asphalt.
Kang et al.[23] prepared ZnO/SBS composite modied as-
phalts through the previously reported methods. It was found that
mother liquor melting is more conducive to the uniform
dispersion of the polymer modier and subsequent stable storage
of the modied asphalt system. However, this preparation pro-
cess is relatively complicated and it was found that the solvent
 C. Fang et al.: J. Mater. Sci. Technol., 2013, 29(7), 589e594
might inuence other properties of the asphalt. Consequently, in
this paper only the high-speed shearing asphalt modication
method which is commonly used in laboratories and in the eld
is summarized.
Considering the cost and nanomaterials dispersion in asphalt,
the content of nanomaterials in the composite should be small. In
addition, the viscosity of asphalt is very large and the compo-
nents are complex, which further increases the difculties of the
nano particle dispersion and diffusion into the matrix[2]. To
reduce the viscosity in preparing the modied asphalt it is
necessary to raise the temperature to facilitate nano particle
diffusion (Brownian motion). Since asphalt is easily aged with
oxygen during the composite preparation, the temperature of the
mixture should not be too high and the shearing time should not
be too long which presents a paradox. Therefore, balancing the
uniform dispersion of nano particles in asphalt and reducing the
aging of asphalt as much as possible will be a key consideration
for future research. Moreover, the particle size of the polymer in
the asphalt is inuenced by the shearing rate and the shearing
time. Polacco[40,41] reported that the polymer swells during
mixing through absorption of the light components of the asphalt
and thus the properties of the base asphalt are altered. As a result,
the swelled polymer particles in the asphalt will also affect the
compatibility of two phases over a certain temperature range,
thus inuencing the modifying effect of the base asphalt.
In the preparation of nano-CaCO3/SBS modied asphalt by
Liu et al.[28], base asphalt was initially melted in 170  C and then
combined with the SBS; the binder was sheared at 170e185  C
at the speed of 4000e6000 r/min. After shearing for 1e1.5 h,
CaCO3 was added and the mixture was sheared for another 1 h at
the speed of 5000e7000 r/min. Next, the binder was swelled at
160e175  C for 2 h yielding the nal asphalt composite product.
Ye et al.[42] used the following process to prepare nano-TiO2/
SBS modied asphalt. Initially, the required dose of SBS was
added and mixed with melted asphalt at 120e130  C and then
cooled for 24 h to ambient temperature. Next, nano-TiO2 was
gradually added to the SBS/asphalt mixture and sheared at a
temperature of about 170  C for 30 min at a high speed of
10,000 r/min, and then held at a temperature of 120  C for
30 min until the modier fully swelled. Finally, modied asphalt
specimen was prepared following another shearing at 170  C,
14,000 r/min for 20 min. The bubbles were excluded from the
mixture by placing the sample in a vacuum oven for about
30 min. Other researchers[8e12,21,23,27e29,33,43,44] reported
different shearing temperatures, speeds and time in preparation
of polymer/nanomaterial modied asphalt and some did not use
the process of swelling. However, Ouyang et al.[30e32], Sure-
shkumar et al.[38], and Polacco et al.[40,41] inserted nanolayered
material into the polymer and prepared a nano/polymer com-
posite master batch and then modied the asphalt with this
composite modier. It was found that this process elicited
different properties from the composite than what occurred using
the normal direct mixing modication method since the com-
posite retained some characteristics of the nano/polymer com-
posite master batch. Therefore, in preparation of nanomaterials/
polymer modied asphalt, use of a master batch and the
sequence of addition of nanomaterials and the polymer will
affect the properties of the modied asphalt.
Considering the different kinds of base asphalt, polymers and
nanomaterials, the preparation process of modied asphalt can vary
dramatically. In addition to these factors, control of the preparation
process parameters such as shearing speed, temperature and time to
591
prepare the modied asphalt with good compatibility and thermal
storage stability are also areas of work for future research in
nanomaterial/polymer multi-modied asphalt.
4. Effects of Nanomaterials on Base or Modied Asphalt and
Their Mechanism
4.1. Compatibility and stability
Compatibility of material is the major factor and the necessary
condition for even dispersion and composite stability. Conse-
quently, researchers are working diligently and using appropriate
technical means to prepare uniform nanomaterials and stably
disperse these in the asphalt matrix. Unfortunately, nanomaterials
can easily aggregate together which causes spot segregation.
This results in the uneven microstructure of the composite
leading to the force eld distortion and nally affecting the
positive aspects of the nanomaterials sometimes resulting in
negative property effects. Lack of dispersion of the added
nanomaterials in a uniform state for extended periods (poor
stability) will cause the microstructure of the composite to
gradually change either during transportation and storage or in
application on a pavement[1]. This condition is unacceptable.
In order to promote the dispersion of Fe3O4 nano particles in
asphalt, Zhang et al.[1] prepared a colloidal system with Fe3O4
nano particles and added this to the melted asphalt and then
prepared modied asphalt using the high-speed shearing method.
It was found that Fe3O4 nano particles can be uniformly
dispersed in asphalt. In addition, benets can be realized from
the effect of surfactants covering the surface of nano particles
which offer a stabilizing effect on the particle electric double
layer and the Brownian motion dynamic stability effect. This
reduced the agglomeration trend of nano particles. In addition,
since asphalt material has a relatively high viscosity, once the
nano particles are uniformly dispersed in the asphalt, the modi-
ed asphalt system has long-term stability and will not spread
coalescence. Xiao and Li[22], Kang et al.[23], Tang et al.[45,46] and
Qu and Pang[47] found that the nano-ZnO can promote even
dispersion of SBS in asphalt. It has long been recognized that
that nanomaterials have special properties such as high surface
area and strong surface free energy and the interface atoms are
arranged in a disordered manner which allows for these atoms to
be bonded to other outside atoms by external forces. Conse-
quently, SBS particles can be adsorbed to the nano-ZnO particles
and their surface free energy is reduced, which reduces the free
energy of the surface of the small particles of SBS, inhibiting the
aggregation of SBS ne particles and improving the binding
capacity of SBS and asphalt interface. As a result, the storage
stability of SBS modied asphalt can be improved.
Huang et al.[48,49] found that a nano bentonite modier offers
unique performance, since it contains 30%e40% isolated freely
dispersed submicroscopic non-agglomerated particles. Once
these particles are mixed with the asphalt they will mutually
exclude each other rather than condense or separate. A strong
interface force can be formed on the surface between the sub-
microscopic non-agglomerated particles and organic solvent, so
the nanolayered silicate particles can be evenly dispersed and
dissolved in the asphalt. Ouyang et al.[30e32] rst prepared sili-
cate nanomaterial/polymer composite and then used it to prepare
modied asphalt. Compared to the base asphalt and polymer
modied asphalt, the particle/polymer modied asphalts
compatibility and thermal storage stability were signicantly
592 C. Fang et al.: J. Mater. Sci. Technol., 2013, 29(7), 589e594
Fig. 2 Fluorescence micrographs of PE modied asphalts without and with OMMT[50].
improved. This is due to the reduction in the difference in density
and polarity between the polymer and asphalt after the polymer
modier had been combined with nanomaterial.
Modied asphalt was prepared with recycled milk bags (the
main component is PE) and OMMT and some encouraging re-
sults were obtained. Fig. 2(a) is the uorescence micrograph of
modied asphalt with 8 wt% recycled polymer showing that the
particle size is uneven, but in Fig. 2(b), the uorescence
micrograph of modied asphalt with 8 wt% recycled polymer
and 2 wt% OMMT showed that PE particles uniformly dispersed
in the base asphalt because the PE molecular chains were
adsorbed by the strong surface energy of OMMT[50].
4.2. Aging resistance
When asphalt is aged, it hardens and becomes brittle and thus
an asphalt roadway will appear to be prematurely damaged.
Asphalt aging is one of the main reasons for pavement
destruction which can be divided into two stages: short term
aging and long term aging. Short term aging is caused by heating
the asphalt in road paving, and long term aging is generated by
the combined action of thermal oxidation, illumination, precip-
itation and the trafc loads in the service life of asphalt pave-
ment[4]. The aging of some modied asphalt includes not only
the aging of the asphalt, but also the degradation of the polymer.
The excellent aging resistance of modied asphalt derived
from its good compatibility and stability, so the compatibility
Fig. 3 Schematic of bitumen-nano clay structure[35].
and stability are the premise of anti-aging properties of the
modied asphalt. In addition, the distribution pattern of the
nanolayered material in modied asphalt also improves the aging
resistance. Zhang et al.[2], Polacco et al.[40] and Yu et al.[51e55]
reported that the exfoliated or intercalated structure of nano-
layered material or polymer modier was formed in the modied
asphalt, as shown in Fig. 3. These structures, especially the
exfoliated one, can produce an effective barrier to oxygen, water
and organic solvents, while preventing the evaporation of the
light components of the asphalt. Therefore, OMMT improves the
aging resistance of modied asphalt, and thus prolongs the ser-
vice life of the modied asphalt pavement. The anti-aging
mechanism of OMMT modied asphalt is shown in Fig. 4.
4.3. Other properties
Other properties of the modied asphalt such as rheology and
pavement performance[56e60] also depend foremost on the
compatibility and stability of modied asphalt. Therefore, all the
factors which affect the compatibility and stability will also in-
uence the other materials properties. We prepared waste-PE/
OMMT modied asphalt with the content of the waste-PE of
8 wt%, and the OMMT contents in modied asphalt samples
1#e5# were 0 wt%, 1 wt%, 2 wt%, 3 wt% and 4 wt%,
respectively[50]. The physical properties indexes of the modied
asphalts are shown in Fig. 5. As can be seen, penetration and
ductility are enhanced with the increase of OMMT content, the
 C. Fang et al.: J. Mater. Sci. Technol., 2013, 29(7), 589e594
Fig. 4 Schematic of anti-aging mechanism of OMMT modied asphalt[51].
stiffness modulus of the asphalt is reduced and the resistance to
deformation is increased. Therefore, the resistance of asphalt
pavement cracking can be improved by mixing waste-PE and
OMMT in the asphalt.
Ye and Chen[15] reported the inuence of TiO2 nano particles
on the high temperature properties of TiO2-modied asphalt. It
was found that the rutting factor and the elasticity of the modied
asphalt were increased, thus the resistance to permanent defor-
mation was enhanced and the service life of modied asphalt
pavement was prolonged. Qu and Pang[47] concluded that a high
specic surface area, super surfactant, and nano particles
strongly absorbed the asphalt, and a special physicochemical
interaction or chemical reaction was resulted[47]. Thus, the light
components in the asphalt were reduced and the asphalt tem-
perature sensitivity was changed. In addition, the pavement
Fig. 5 Physical properties indexes of modied asphalt.
593
performance of nano particle-modied asphalt concrete was
enhanced.
In the research of SiO2/SBR modied emulsied asphalt,
Chen et al.[29] found that the addition of nano-SiO2 caused an
improvement in comprehensive properties of the base asphalt.
During the heating process, the liquid phase was reduced and
changed to solid phase resulting from the effects of the network
structure formed by the nano-SiO2 physical cross linking points
and SBR. The swelling of SBR after absorbing the oil in asphalt
was the main reason for the improvement in the properties of
modied asphalt[29]. Tang and Han[46] proposed that nano par-
ticles played a special role in physical and chemical properties of
the composite due to the small size of polymers, nonpaired atoms
in the surface and the good ability to be combined with poly-
mers. The toughness of nano/polymer composite was enhanced
and the good rigidity and strength of the polymer were main-
tained. This indicted a new direction for the application of
modied asphalt and it is expected to develop and produce a
nano silicate/polymer/asphalt material with high strength, high
toughness, high temperature resistance, aging resistance and
water resistance[46].
5. Conclusions and Perspectives
Throughout the eld of modied asphalt with nanomaterials,
different nanomaterials appear to play a positive role in improving
the properties of asphalt. Mechanisms of using nanomaterials
together with the base or polymer modied asphalt and the nano/
polymer/asphalt system from various perspectives have been sum-
marized and analyzed. As more investigators pay attention to the
nanomaterials applied in asphalt modication, nanoscience and
nanotechnology will help make greater progress in asphalt modi-
cation. In the preparation of the modied asphalt, conventional
polymer modied asphalt preparation methods have been used, but
the inuence of various preparation process parameters, such as
temperature, shearing speed and time on the modied asphalt
product has not been investigated. It is believed that the modication
of nanomaterials on base asphalt or modied asphalt is a chemical
reaction process. Methods for introducing a reasonable dose of nano
particles into the asphalt to achieve nanoscale dispersion and
improve the compatibility of every phase and the comprehensive
properties of the modied asphalt materials will be the focus of the
research work in this eld. Simultaneously, further research on the
mechanism of nanomaterials modied asphalt and its microstructure
will be signicant in guiding engineering practices.
594 C. Fang et al.: J. Mater. Sci. Technol., 2013, 29(7), 589e594
Acknowledgments
The authors acknowledge the nancial supports from the
National Natural Science Foundation of China (Grant Nos.
51002118 and 51172180), Program for New Century Excellent
Talents in University of Ministry of Education of China (Grant
No. NCET-12-1045) and Shaanxi Programs for Outstanding
Youth Project (2011).
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