Construction and Building Materials 330 (2022) 127222

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Construction and Building Materials

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

Review

A review on Graphene/GNPs/GO modified asphalt

Junxi He a, Wei Hu b, Rui Xiao b, Yanhai Wang b, Pawel Polaczyk b, Baoshan Huang b, *
a
The Key Laboratory of Road and Traffic Engineering of Ministry of Education, Tongji University, Shanghai 201804, PR China
b
Department of Civil and Environmental Engineering, the University of Tennessee, Knoxville, TN 37996-2313, USA

A R T I C L E I N F O A B S T R A C T

Keywords: Two-dimensional (2D) materials such as graphene, graphite nanosheets (GNPs), and graphene oxide (GO) are
Graphene frequently used in the areas of biology, electronics, environment, etc. In recent years, increasing attention has
Graphite nanosheets been paid to the application of these materials in pavement engineering. This paper summarizes the progress and
Graphene oxide
challenges of using graphene-like materials in asphalt binder and asphalt mixture. The major conclusions are as
Asphalt binder
follows: 1) The graphene-like materials can improve the high temperature performance, moisture stability, aging
Modification mechanism
resistance, and skid resistance of asphalt binder, but the effect on low temperature performance depends on the
dispersion of graphene-like materials in asphalt binder; 2) The effect of graphene-like materials on the surface
texture of aggregate in asphalt mixture needed to be further verified; 3) The three methods for the preparation of
modified asphalt were summarized: the direct addition method (DAM), the indirect addition method (IAM), and
the auxiliary addition method (AAM). Among them IAM and AAM can reduce the usage of graphene-like ma­
terials and improve their dispersion in asphalt binder; 4) Only physical reactions exist in the system of graphene
modified asphalt (GMA) and graphite nanosheets modified asphalt (GNMA). In the system of graphene oxide
modified asphalt (GOMA), the existence of chemical reaction needs to be further verified; 5) The modification
mechanism was explained by both the substitution effect hypothesis (SEH) and the intercalation structure hy­
pothesis (ISH).

1. Introduction stability, response speed (~30 ms and ~ 50 ms, respectively) and

controllable sensitivity. M. Krystek, et al. [12] reported that the cement-
Since the discovery of graphene materials in 2004[1], various 2D based materials were modified via adding the exfoliated graphene (0.05
materials have gained significant attention in recent years such as the wt%) directly, in which the tensile strength (~79%), compressive
boron nitride (BN), molybdenum disulfide (MoS2), tungsten disulfide strength (~8%) and Young’s modulus (~9%) were improved to a certain
(WS2), and also their derivatives [2–4]. Among these various 2D mate­ extent. Meanwhile, graphene could also promote the hydration reaction
rials, graphene, a single-layer carbon sheet with hexagonal stacked in this system. Based on the flexible surface of GO, H. Cheng, et al. [13]
lattice structure, has many unique properties such as high carrier prepared a flexible in-plane moisture-electric converter for non-contact
mobility at room temperature (~15000 cm2/V⋅s) [1], high specific interaction mode. Y. Su, et al. [14] prepared a multilayer graphite
surface area (~2600 m2/g) [5], strong thermal conductivity (3000 ~ barrier based on GO to improve the barrier effect on various molecules.
5300 W/m⋅K) [5], good light transmittance (~97.7%) [6], high Young’s D. Quan, et al. [15] added GNPs to the epoxy adhesive to improve its
modulus (~1tPa) [7], etc. Therefore, graphene and its derivatives (such young’s modulus (2.46GPa up to 2.56GPa), colloidal fracture energy
as graphite nanosheets (GNPs), and graphene oxide (GO)) has been (~21%) and folding shear strength (~21.7 MPa). B. Wang, et al. [16],
investigated for various applications in electronics, information, energy, reported that GNPs could improve flexural strength of the cement-based
materials, environment, biology and many other fields. Y. Qiao, et al. [8] materials and decrease the total porosity of those.
and P. Snapp, et al. [9] reported that the electronic skin and photo­ In general, graphene, GNPs and GO are widely used in flexible de­
electric sensor were produced via graphene for the human health vices, medical detection, intelligent systems and composite materials
monitoring, respectively. A new flexible capacitance sensor has been [17–25]. Because of its excellent performance, graphene and its de­
developed by J. Yang, et al. [10] and S. Luo, et al. [11], which has good rivatives once were regarded as a universal material. It seemed that any

* Corresponding author.
E-mail addresses: [email protected], [email protected], [email protected] (B. Huang).

https://doi.org/10.1016/j.conbuildmat.2022.127222
Received 31 December 2021; Received in revised form 23 February 2022; Accepted 17 March 2022
Available online 24 March 2022
0950-0618/© 2022 Elsevier Ltd. All rights reserved.
J. He et al. Construction and Building Materials 330 (2022) 127222

material or structure could be rebuilt and improved with it. Therefore, material and is composed of various complex compounds [70–72].
its application in pavement engineering was also investigated. A pri­ Adding graphene maybe lead to different modification mechanism and
mary issue in pavement engineering is the mismatched performance of performance improvement effects. Meanwhile, the exploration of its
the original base asphalt corresponding to heavy traffic or severe modification mechanism is also relatively difficult. So, the purpose of
weather [26–32,162]. At present, there are a wide range of asphalt this review is to summarize the effect of graphene-like materials on
modifiers, such as rubber, resin, high molecular polymer, inorganic salt, asphalt binder and to explain the modification mechanism, via the
etc., in optimizing the performance of the base asphalt [33–37]. How­ existing related studies.
ever, the existing modifiers have a common unsolved challenge, that is,
when the modifier improves the low-temperature performance of 2. Review significance
asphalt, its high-temperature performance will usually be impaired,
such as polyethylene, polypropylene [38–42], and vice versa, such as The performance modification of asphalt binder with using
polyethylene fiber, styrene butadiene rubber (SBR) [43–46]. graphene-like materials has been widely studied by researchers.
Because of the disadvantages of traditional modifiers, the modifiers Compared with traditional modifiers, such as resin, rubber, thermo­
prepared via nanomaterials and their derivatives were gradually plastic rubber, fiber, etc., it was found that, on the one hand, the size of
explored and applied. As another kind of carbon-based nanomaterials, the graphene-like materials belongs to nanoscale, which made it very
carbon nanotube (CNT) is like a cylinder in shape, whose tube is difficult to characterize the morphology of materials in asphalt binder;
composed of a single layer of carbon atoms [47–49]. Its mechanical and on the other hand, its properties were very complex, such as ultra-high
chemical properties are similar to those of graphene, but there are still specific surface area and ultra-high Young’s modulus, which made it
differences due to their different structures from those of graphene or very difficult to explain its modification effect and mechanism. Ac­
graphene derivatives [50–52]. During the preparation process of CNT cording to the existing literature on the modification of asphalt binder
modified asphalt, some CNTs’ morphology were damaged and the pipe based on graphene-like materials, the evaluation of the modification
wall were expanded, which was similar graphene-like materials and effect for these graphene-like materials was ambiguous, that is, some
provide the reference for the research of graphene-like materials researchers believed that the graphene-like materials could compre­
modified asphalt. A.A. Mamun, et al. [53] reported that the water sta­ hensively improve the high- and low-temperature performance of
bility of styrene butadiene (SB) and styrene butadiene styrene (SBS) asphalt binder and had a great application prospect, whereas another
could be improved via adding 1.0% and 1.5% CNT, respectively. researchers believed that these materials could not have a substantial
Meanwhile, CNT could improve the storage stability [54], the structural impact on the performance of asphalt binder, so it is not worthy of
stability [55], the fatigue resistance [56], high-temperature perfor­ further research in this field. Moreover, there was no detailed and clear
mance, and low-temperature performance [57] of SBS modified asphalt. explanation for preparation parameters and modification mechanism.
P. K. Ashish, et al. [58] reckoned that the content of CNT should not Therefore, in this review, the graphene-like materials were selected as
exceed 1.5%, otherwise it was easy to cause agglomeration. Besides the research focus to explore preparation parameters of modified
CNT, other nanomaterials were also gradually used in the field of asphalt, their influence on the performance of asphalt, their modifica­
modified asphalt binder. J. Jin, et al. [59] reported that nano organic tion mechanism. The final purpose of this paper is to provide an
palygorskite could improve the water stability and high temperature important reference for 2D material modified asphalt.
stability of SBS modified asphalt with only adding 3 wt%. C. Zhu, et al.
[60] reported that a composite modifier prepared by 3% nano-zinc oxide 3. Potential relationship
and 1% organic expanded vermiculite could improve the aging resis­
tance of the SBR modified asphalt. F. S. Bhat, et al. [61] believed that Asphalt, kerosene or petroleum by-products, can not only be used as
nano Al2O3 could improve aging resistance and high temperature per­ road pavement materials, but also as carbon precursor materials [73,
formance of SBS modified asphalt with only adding 4 wt%. H. Yao, et al. 150–161]. There are many hydrocarbons with different molecular
[62] compared the modification effects of carbon microfiber, nanosilica, weight in asphalt binder. In addition, asphaltene, aromatics and other
non-modified nanoclay and polymer modified nanoclay on asphalt and substances have stable benzene ring structure composed of carbon atoms
the non-modified nanoclay had the best effect. It can be seen from the [74–75]. Similarly, graphene, GNPs and GO are carbon based materials,
above that nanomaterials can affect the performance of asphalt with a which also have the same structure [76]. I. F. Cheng, et al. [77] reported
very small amount. Moreover, graphene and graphene derivatives have that the carbon film was formed via heating asphalt and condensing
more excellent mechanical and electrochemical properties than the asphalt smoke into the inner wall of ceramic, whose structure was
above nanomaterials, which meant that graphene-like materials could multilayer GNPs. The preparation principle was shown in Fig. 1 (a). T. S.
be a better modifier for asphalt binder. In fact, graphene-like materials sreeprasad, et al. [78], using asphalt and fine sand as raw materials,
have been the most studied object in the research field of nanomaterials through in-situ synthesis method as shown in Fig. 1 (b), graphene-sand
modified asphalt. composite with super adsorption capacity was formed on the surface of
Due to their unique properties, using graphene and its derivatives to fine sand, as shown in Fig. 1 (c, d, e), with asphalt content of 0.5%, 1%
modify asphalt materials has the potential to overcome other modifier’s and 1.5% respectively. The material can absorb the impurities in the
issue. However, unlike the electronic, information and medical in­ sewage, which has an important reference for the purification of sewage.
dustries, the amount of materials used in pavement industries is enor­ W. Yang, et al. [79] reported that carbon nitrided GNPs were combined
mous. The utilization of graphene and its derivatives in pavement with petroleum asphalt to prepare one kind of super-capacitor with high
industry can only be based on their large-scale and industrialized pro­ capacitance and good stability. This also showed that the modified
duction [63–66]. B. Zhang, et al. [67] reported that via using renewable asphalt may had the effect of capacitor, and its structural principle is
glucose and cheap ferric chloride as raw materials, high-quality gra­ shown in Fig. 1 (f). K. Zhang, et al. [80] reported that GNPs modified by
phene was prepared on a large scale and cheaply with chemical vapor NiFe2O4 were coated with asphalt materials, and the synthesized ma­
deposition method. T. F. Emiru, et al. [68], provided important basis for terials had the properties of ultra-high microwave absorption. R. Wang,
the large-scale preparation of GO via using potassium permanganate and et al. [81] reported that amino functionalized graphene was successfully
ascorbic acid as catalyst. As early as 2010, Z. Wang, et al. [69], had synthesized from petroleum asphalt with high softening point and
realized that the large-scale production of GNPs could be achieved by ammonia water, which could be used as a fluorescent sensor to detect
arc evaporation method. These studies revealed that industrialized and monitor Fe3+ ions effectively. Y. Li, et al. [82] reported that gra­
production of graphene and its derivatives is feasible. phene was successfully prepared from petroleum asphalt as carbon
In addition, unlike polymer materials, asphalt is a type of viscoelastic source via pulsed arc discharge method in water. Meanwhile, hydrogen

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J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 1. (a) is the graphene deposition apparatus. Reproduced with permission from ref. [77], Copyright 2019, Elsevier. (b) is the schematic illustration of the
formation GSC. (c,d,e) are the SEM image of GSC with 0.5, 1, 2% of asphalt, respectively. Reproduced with permission from ref. [78], Copyright 2013, Elsevier. (f) is
the schematic diagram of the combination of carbon-nitrided graphene and petroleum asphalt. Reproduced with permission from ref. [78], Copyright 2019, ACS
Publications. (g) is the simulation of the conversion process from asphaltene to 3D graphene. (h,i) are the SEM image of 3D graphene. Reproduced with permission
from ref. [83], Copyright 2014, Elsevier. (j) is the illustration of the synthesis process of graphene from asphalt adsorbed via vermiculite. (k) is the carbonization
mechanism of asphalt with different combination methods. Reproduced with permission from ref. [86], Copyright 2013, Elsevier.

was produced in the process of graphene formation from asphalt. Most relationship between graphene and asphaltene. P. Zhao, et al. [87]
of its layers’ number were 2 ~ 5, and a few were 5 ~ 10. Z. Liu, et al. synthesized high-quality graphene quantum dots, i.e., a kind of gra­
[83] also reported that using asphalt as carbon source, the three- phene material with fluorescence reaction, via using oxidized deoiled
dimensional graphene was synthesized on the nickel foam via vapor asphalt as raw material by microwave method. S. Yang, et al. [88] re­
deposition method, which was a single layer graphene hetero-structure, ported that high-quality graphene was prepared via ultrasonic stripping
and the number of structure layers was similar to that of [82], that is, in sulfonated asphalt solution. The ID/IG value was only 0.331, and the
most of which were 2 ~ 5 layers, and a few parts exceeded 5 layers. The value could be decreased with the increase of the concentration of sul­
synthesis mechanism of graphene prepared by asphalt was simulated, as fonated asphalt solution.
shown in Fig. 1 (g), and the three-dimensional structure of graphene was To sum up, the above literature showed the research on the prepa­
shown in Fig. 1 (h, i). Y. Xie, et al. [84] and Fernández, et al. [85] had ration of graphene, GNPs and GO based on petroleum asphalt as carbon
successfully synthesized graphene from petroleum asphalt via thermal precursor. Therefore, it can be seen that there was a close relationship
decomposition reaction. The former also thought that sulfur played an between this type of graphene-like materials and asphalt binder. In
important role in the formation of graphene. The latter thought that the addition, these studies also showed that graphene, GNPs and GO had the
conversion efficiency and production of graphene materials were greatly possibility of stable existence or interaction in asphalt, which also pro­
improved and the production cost was also reduced via this method. C. vided a theoretical basis for the preparation of modified asphalt.
Xu, et al. [86] considered that asphaltene in asphalt had polycyclic ar­
omatic hydrocarbon structure. Through catalytic rearrangement of the 4. Preparation method
polycyclic aromatic hydrocarbon structure of asphaltene on the surface
of vermiculite layer, graphene was synthesized with 8 ~ 10 layers. The According to the relevant literature, the preparation methods and
synthesis principle diagram is shown in Fig. 1 (j). And it was considered parameters of nanomaterials modified asphalt will have corresponding
that under irregular stacking and arrangement, asphalt macro-molecules differences based on different modifier types [89–91]. Based on 2D
formed petroleum coke and under regular arrangement and distribution, materials such as graphene, GNPs and GO, the preparation parameters
these formed graphene fragments. The principle is shown in Fig. 1 (k). In and methods may be different from those of traditional modified
addition, the capacitance prepared by this graphene had higher capac­ asphalt. Therefore, this paper summarized and analyzed the preparation
itance. This provided evidence support for the transformation parameters and methods of graphene-like materials modified asphalt, as

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J. He et al. Construction and Building Materials 330 (2022) 127222

shown in Table 1 and Fig. 2. form a solution at room temperature, and the two solutions were evenly
According to Table 1 and Fig. 2, the preparation process and pa­ mixed. Finally, the medium solution was separated from this system, so
rameters of graphene, GNPs and GO modified asphalt can be roughly as to achieve the purpose of uniform dispersion of graphene-like mate­
divided into three categories. The first type is direct addition method rial modifier. Similarly, R. Yu, et al. [131] also reported that GO aqueous
(DAM), that is, adding graphene-like materials directly into asphalt; The dispersion was prepared firstly, that is, GO was fully and evenly
second type is indirect addition method (IAM), that is, asphalt binder dispersed in the solution system, then the aqueous dispersion was fully
and graphene-like materials are both dissolved in the medium solution mixed with molten asphalt, and finally the aqueous solution was evap­
to form a solution and mix them, with a purpose of uniform dispersion of orated to obtain GOMA. It was worth noting that as the medium solu­
graphene-like materials in asphalt; The third type is auxiliary addition tion, it needed to be able to convert asphalt binder and graphene-like
method (AAM), that is, graphene-like materials are modified by func­ materials into liquid at room temperature without affecting their basic
tional groups and then added into asphalt binder. By analyzing the use properties. It was thought that the above preparation method fully
frequency of the instrument, it is obvious that the use frequency of high- considered the uniform dispersion of the graphene-like materials in the
speed shear instrument in the preparation of GMA and GNMA is asphalt medium. Obviously, the mixture of two types of liquid will be
significantly higher than that of GOMA. And when other additives are more evenly dispersed than that of solid and molten. It also provides a
added, the frequency of high-speed shear apparatus will also increase. It new idea for the preparation of 2D material modified asphalt, which has
is speculated that graphene and GNPs are more difficult to disperse in important reference significance.
asphalt binder than GO. Because GO has oxygen-containing functional
groups, it can be prepared by ordinary glass rod stirring at a relatively 5. Influence of 2D materials on asphalt
high temperature. It is worth noting that when preparing modified
asphalt in ref. [97,100,101,112,131,137,138], ultrasonic dispersion in­ 5.1. Influence of Graphene
strument was used to conduct ultrasonic treatment on graphene-like
materials or modified asphalt, so as to increase the dispersion of 5.1.1. Macro influence
graphene-like materials in asphalt binder. Meanwhile, in the ref. As a new 2D material, graphene was defined in the form of mono-
[96,97,100,101,107,110,111,112,113,114,128], surfactant was used to layer at the beginning. In the vertical dimension, each layer of gra­
modify the basic properties of graphene-like materials via grafting phene has only the height of a single carbon atom, which is composed of
functional groups. The main purpose is to improve its affinity in asphalt six carbon atoms to form a benzene like ring structure, and the honey­
materials, increase its dispersion, make it evenly dispersed in asphalt comb structure is formed in turn. However, with the extensive research
binder, and give full play to its modification effect. G. Huang, et al. [101] and development of graphene composites, in order to facilitate the
prepared the modified asphalt differing from other literature. The gra­ research and development of composites and determine the properties of
phene modifier was prepared into a uniformly dispersed solution, and composites, the definition of graphene layer number has been expanded
then trichloroethylene and other solvents were used to make the asphalt from the original definition of 1 layer to 1 ~ 10 layers, which can be

Table 1
Summary of literature on preparation parameters of GMA/GNMA/GOMA.
Preparation apparatus Mixing parameters
Material
Ref. additives High speed Temperature Types
pretreatment Agitator Others Time/min Speed/r.p.m.
shearer /◦ C

[93] × × × √ × (10)* Manual stirring 150 GMA

[96] √ √ √ √ × 10/30/(10)** 1000/3000** 145 ~ 155**
[97] √ √ √ × √ 180 6500 140
[99] × × √ × × 60 1720 140
[100] √ √ × √ × (1 2 0) (4 0 0) 165
[101] √ √ √ × √ 120 4700 110
[103] × √ √ × × 120 3000 135
[107,110,111] √ √ √ √ × 40/(60) 5000/(5 0 0) 170 GNMP
[112] √ √ √ √ √ 40/40/(30) 5000/160/(3 0 0) 135
[113] √ √ √ √ × (15)/45 unknown 175 ~ 185
[114] √ √ √ √ × 40/(80) 5000/(5 0 0) 170
[115] × × × √ × (10) Manual stirring 150 ~ 160
[117] × × × √ × (6 ~ 40) Manual stirring 165
[118] × × √ × × 60 3000 unknown
[122] × × × √ × unknown Manual stirring 135 GOMA
[123] × × √ × × 30 4000 155/170***
[124] × × √ × × 45 unknown 150/160
[125126] √ × × √ × (45/60) Manual stirring 150/135
[127] √ × × √ × (45/20) Manual stirring 160/130
[128] √ √ √ √ × 30/(60) 5000/(4 0 0) 170
[131] × × × √ √ unknown Manual stirring 150
[132] × × √ × × 30 4000 150
[133] √ √ √ √ × 40/(60) 5000/(5 0 0) 170
[134] √ × × √ × unknown Manual stirring 170 ~ 190
[135] × × √ × × 45 2000 155
[137138] × × √ × √ 45 5000 120
[139] × × √ × × 45 3000 165

Notes: *The parameters outside the brackets are the preparation parameters of high-speed shear, while the parameters inside the brackets are the preparation pa­
rameters of agitator or manual stirring.
**
“10/30/(10), 1000/(3000), 145 ~ 155” means that the preparation temperature is 145 ~ 155 ◦ C and the modified asphalt was prepared via firstly, high speed
shearing at 1000 r.p.m. for 10 min, then shearing at 3000 r.p.m. for 30 min, and finally stirring for 10 min. Similarly hereinafter.
***
“155/175” means that the graphene-like materials modified asphalt were prepared with two kinds of asphalt binder, and the preparation temperatures were 155
and 175 ◦ C, respectively.

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J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 2. The summary of preparation methods of 2D material modified asphalt.

called graphene [92]. Table 2 summarizes a series of studies on gra­ simulate and analyze the thermodynamic properties of GMA. It was
phene used in modified asphalt in recent years. believed that the addition of graphene can significantly improve the
According to the relevant literature in Table 2, F. Moreno-Navarro, glass transition temperature of modified asphalt, that is, improve its
et al.[93] thought that the addition of graphene could reduce the high temperature stability. However, glass transition temperature is
phase angle of asphalt. If the content of graphene was higher, the phase often used to characterize the high- and low-temperature properties of
angle could be reduced by 10%, and the elastic properties and thermal single or single compounds [104–106]. Because asphalt binder contains
conductivity of asphalt could be also increased. Meanwhile, although complex compounds, it is questionable to judge the high temperature
the asphalt binder with graphene was easier to be heated than the performance of modified asphalt directly via this parameter. In addition,
asphalt binder without graphene and the temperature rose faster for the it was considered that the addition of graphene can also improve the
asphalt binder with graphene, it had stronger high temperature stability shear modulus G, bulk modulus E and Young’s modulus K of asphalt, and
and was not easy to deform. The optimum content of graphene was 0.5 make the thermal expansion coefficient of modified asphalt greater than
~ 1.0%. M. A. Nazki, et al.[99] also carried out the rheological analysis that of base asphalt, which indicated that the volume deformation of
and heat conduction analysis of GMA. It was believed that graphene GMA was not easy to occur after being heated. It was consistent with the
could reduce the phase angle and decrease the modulus of asphalt relevant test results in ref. [93]. However, the optimum content of
binder, and increased the thermal conductivity of asphalt binder graphene was 10.6% via simulation method, which was different from
(increased by 50 ~ 80%), which was similar to the research results in that of the ref. [93,100].
ref. [93]. It is also considered that graphene could improve the rutting X. Zhang, et al.[97] reported a new method to determine the opti­
resistance and multi-stress creep recovery rate of asphalt binder, but the mum content of graphene which was modified by Ethylene Bis-
effect on the complex modulus of asphalt at high temperature (increased Stearamide (EBS). Through the uniform design method, the prepara­
by 92.40% at 65 ◦ C) was much greater than that at low temperature tion parameters, graphene content, surfactant content and other pa­
(increased by 10.94% at 25 ◦ C). rameters were taken as the effect factors, and the performance index of
T. Guo, et al. [96] reported that the mixture of graphene and tour­ GMA was taken as the reference standard to establish the relevant
maline in the ratio of 1:100 was used as a composite modifier to modify model, which was verified by theory and experiment. It was considered
asphalt. They found that the composite modifier could significantly that graphene can improve the stability of matrix asphalt at high tem­
improve the rheological properties of asphalt binder, and improve the perature, based on the improvement of softening point (21.83%), rutting
rutting resistance of asphalt binder, up to 10.12%. It was also considered resistance factor (45.54%), creep recovery rate of 0.1kpa (824.2%).
that the asphalt molecules may enter the graphene structure, making the Similarly, it can also improve its low temperature stability, based on the
two more closely combined, so as to improve the performance of increase of 5 ◦ C fracture energy (940.93%). The results showed that the
asphalt. The composites of graphene and tourmaline were also used by best content of graphene was 0.2%, and the surfactant EBS content was
Q. Chen, et al. [94]. The mixture of graphene and tourmaline could 1%. Moreover, G. Huang, et al. [101] reported that the material
replace mineral powder to improve the high temperature stability of composition model of graphene solution modified by surfactants
asphalt mixture, but its low temperature stability and water stability had dipropylene glycol dimethyl ether (DME) and polyvinylpyrrolidone
no obvious change. It’s another main function was to absorb the asphalt (PVP) was established based on UV/Vis spectrophotometry and Lambert
smoke released by hot asphalt, and its absorption and emission reduc­ Beer’s law, which can make graphene more evenly dispersed in the
tion efficiency reached 76.9–80.5%. However, the method of testing asphalt binder. The optimum contents of graphene were 0.26% and
asphalt smoke is questionable. It can extract the asphalt smoke solution 0.53%, respectively, based on surfactant PVP and DME. Through the
by absorbing asphalt smoke, whose main component was polycyclic preparation method IAM, GMA was prepared. It was considered that
aromatic hydrocarbons (PAHs), but also contained a small amount of graphene can effectively improve the high temperature stability of base
sulfur heterocyclic compounds and oxygen containing aromatic com­ asphalt, based on the increase of softening point (7.17%, 4.57%), 0.1
pounds, and the absorption peak at 280 nm was used to judge the kPa creep recovery rate (867.88%, 646.77%), 3.2 kPa creep recovery
emission reduction efficiency. According to reference [101], graphene rate (153.53%, 128.62%) and anti-rutting factor (40.51%, 17.26%), and
still has an absorption peak at 280 nm, meanwhile graphene has strong the decrease of 0.1 kPa non-recoverable compliance (30.95%, 20.82%)
adsorption capacity, which may exist in the released PAHs. The method and 3.2 kPa non-recoverable compliance (18.88%, 8.63%). Similarly,
needs to ensure that the extracted asphalt smoke solution does not the low temperature stability of base asphalt is also improved, based on
contain graphene in order to reflect its effectiveness, which needs to be the increase of fracture energy (98.81%, 55.51%) and ductility (18.30%,
further studied. X. Zhou, et al. [95] used molecular dynamics method to 14.91%).

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J. He et al. Construction and Building Materials 330 (2022) 127222

X. Zhang, et al.[102] reported that graphene was directly used to

[100]

[101]

[102]

[103]
modify base asphalt without surfactant. It was found that graphene can

[93]

[96]

[97]

[99]
Ref.
still improve the softening point, multi-stress creep recovery rate, anti-
rutting factor, and the viscosity of base asphalt, which was consistent

Graphene could increase the viscosity of base asphalt. The interlayer distance of graphene was enlarged
Graphene could change the rheological properties of asphalt. The optimum content of graphene may be

Graphene was modified by surfactant PVP and DME. Material composition model of graphene solution
Polyacrylonitrile fiber could be modified via graphene in dopamine solution. Graphene could improve
Graphene reduced the phase angle of asphalt and increased its elasticity and thermal conductivity. The

was established. The optimum contents of graphene were 0.26% and 0.53%, and those of surfactant PVP
Graphene could improve the thermal conductivity of asphalt. The optimum content of graphene was
Graphene was modified via surfactant EBS. The optimum content of graphene was 0.2%, and that of
with the relevant results in ref. [97,101]. But the ductility was decreased

Graphene could improve the viscosity and aging resistance of base asphalt. The optimum content of
and not improved. It was considered that this phenomenon may be
caused by the modification of surfactant. The amount of graphene
modified by surfactant can be significantly less than that of unmodified

the water stability, low temperature flexibility and crack resistance of asphalt mixture.
graphene, and the modification effect was better, which can be seen that
the surfactant was conducive to the dispersion effect of graphene in
asphalt materials.
M. Shishebor, et al. [98] used molecular dynamics method to simu­
late the adhesion work and strength of interface between graphene and
asphalt, and that of graphene and aggregate. It was considered that the
adhesion work and strength of graphene-aromatic hydrocarbon and
graphene-asphaltene were greater than that of graphene-saturate, and
the highest adhesion work and strength could reach 220mj/m2 and
1400 MPa, the former was almost 30% higher than the latter. And the
and DME were 190% and 160% based on graphene.

average adhesion work and strength of graphene-asphalt were 133%

optimum content of graphene was 0.5 ~ 1.0%.

and 150% higher than that of graphene-aggregate, respectively. Gra­

phene had little contribution to the adhesion of aggregate. It was
surfactant was 1% based on graphene.

considered that graphene mainly acted on aromatics and asphaltene in

asphalt, and also had a certain effect on resin, which provided a good
basis and direction for the follow-up experimental verification and
mechanism analysis.
Z. Su, et al.[100] reported that the polyacrylonitrile fiber was
modified via covalent grafting with graphene in dopamine medium, and
graphene was 1%.
more than 0.3%.

then the modified asphalt was further prepared. It was considered that
by asphaltene.
Other findings

1.0 ~ 1.5%

the viscoelasticity, deformation resistance and water resistance of the

modified asphalt were greatly improved after adding graphene, and the
temperature sensitivity was reduced. Based on this modified asphalt, the
water stability and bending resistance of asphalt mixture were also
improved. Interestingly, it was believed that graphene can improve the
modulus
Storage

loss modulus of modified asphalt to some extent, which was inconsistent

with the relevant conclusions in ref. [93,96,99]. The authors thought
–

that the reason may be caused by polyacrylonitrile fiber, not necessarily

modulus

caused by the effect of graphene.

Loss

X. Li, et al.[103] analyzed the aging resistance of GAM via rolling

–

thin film oven test (RTFOT) aging and pressurized aging vessel (PAV). It
Recovery

was found that graphene can effectively improve the aging resistance of
base asphalt, and it was believed that the reason was the increase of
rate

viscosity of base asphalt and the effect of graphene sheet blocking ox­
–

ygen molecules to enter the asphalt system. Meanwhile, it was consid­

Rutting
factor

ered that graphene played the role of micelle binding in asphalt binder
due to its high surface energy, and the uniformly dispersed graphene can
replace the role of asphaltene.
Ductility

5.1.2. Micro influence

–

–
Summary of literature on the effect of graphene on asphalt.

According to the literature, the micro characterization and simula­

tion results of GMA are shown in Fig. 3 and Fig. 4.
Softening

According to Fig. 3 (a ~ d), F. Moreno-Navarro, et al. [93] analyzed

point
Effect of Graphene

the thermodynamic properties of GMA via infrared camera. When gra­

–

phene is added into asphalt material, the heat conduction performance

Penetration

of asphalt material can be significantly improved, that is, when the same
temperature difference is increased or decreased, the time is shorter. It
seems that the temperature sensitivity of GAM will increase. However,
–

Fig. 3 (a, b) showed that the GMA was more stable and less prone to
deformation than the base asphalt at the same temperature. The authors
increment of 0.2%

0.1, 0.2, 0.3, 0.4,

0.1, 0.3, 0.5, 0.7

believed that the research results can provide a good research basis and
0.5, 1, 1.5, 2.0
0.2 ~ 2 at an
0.1, 0.2, 0.3

thinking direction for the follow-up research of intelligent pavement

0.1, 0.5, 1

0.5, 1.0, 2

0.5, 1, 1.5
dosage/%

0.5 (PVP)
Graphene

materials. For example, graphene can be used to increase the specific

(DME)
1, 2, 3

heat capacity of asphalt materials, which can effectively absorb the

energy stored on the road, and use the energy transmission pipeline to
transfer it to the heat energy conversion station for energy conversion,
64–22
B 50/70

VG40
SK-70#

SK-70#
Table 2

VG30/
Binder

AH-70

AH-70

and graphene can greatly improve the effectiveness and efficiency of this
A-70
type

PG

process. Moreover, it can also be used in the development of snow-melt

6
J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 3. (a, b) are the experiment to determine the heating capacity of the GMA. (c, d) are the experiment conducted to evaluate the thermal conductivity of the GMA.
Reproduced with permission from ref. [93], Copyright 2018, Elsevier. (e, f) are the dispersion of graphene/tourmaline in asphalt and morphology of composite
powder. Reproduced with permission from ref. [94], Copyright 2020, Elsevier. (g) is the interface model representation of Graphene-SARA. (i) is the interface model
representation of Graphene-SiO2. (h) is the adhesion properties of Graphene-SARA and Graphene-SiO2. Reproduced with permission from ref. [98], Copyright 2019,
Taylor & Francis Group.

pavement and the research and development of high temperature sta­ the agglomerates was larger. By contrary, when the content of graphene
bility of pavement in tropical or subtropical regions, that is, through its was the best, the agglomeration phenomenon in asphalt binder would be
high thermal conductivity, the high temperature of pavement will be improved, and the agglomerates was gradually smaller. It was proved
transferred to the outside of the pavement to reduce the impact of high that there was an optimal amount of graphene in asphalt binder, and its
temperature on pavement performance. parameters would seriously affect the dispersion of graphene in asphalt
Fig. 3 (e) showed the SEM morphology of graphene-tourmaline binder. The addition of surfactant could effectively improve the
composite in asphalt binder, and Fig. 3 (f) showed the SEM agglomeration phenomenon of graphene. However, it is not explained
morphology of the interaction between graphene and tourmaline. Q. how the surfactant acts on graphene. Similarly, according to Fig. 4 (c ~
Chen, et al. [94], via using this composite effectively, the amount of f), G. Huang, et al. [101] also reported that the 3D and 2D morphology of
asphalt smoke emission was reduced, and this reduction effect was far graphene in asphalt binder via means of metallographic microscope and
greater than that of tourmaline alone. Fig. 3 (g ~ i) showed that M. industrial CT, and analyzed the relationship of dispersion of graphene
Shishebor, et al. [98] used molecular dynamics method to simulate and agglomerates in asphalt binder between 2D and 3D image, and
analyze the interaction effect between graphene and four components of confirmed that surfactant can effectively increase the distance between
asphalt binder and between graphene and aggregate. Obviously, the graphene sheets via industrial CT scanning, which was about twice the
adhesion work and interface strength of graphene-asphalt were much original distance. According to Fig. 4 (g, h), X. Zhang, et al. [102] re­
greater than that of graphene-aggregate. The authors thought that this ported that the morphology of expanded graphite which was separated
conclusion provided a certain research basis for the subsequent study of from hot expanded graphite modified asphalt was similar to that of
GMA mixture. However, the interaction of the interface between GMA graphene. It was believed that some substance in asphalt binder exfo­
and aggregates considered not only the effect of interface between liated expanded graphite to form graphene-like substance. Meanwhile, it
graphene and aggregate, but also other factors. was considered that the morphology of asphaltene was similar to that of
According to Fig. 4 (a, b), X. Zhang, et al. [97] showed the graphene, and this process may be caused by the action of asphaltene.
morphology of graphene in asphalt binder via means of metallographic Fig. 4 (i) showed that the simulation results of the interaction between
microscope. When the content of graphene was not the best, the asphaltene and graphene. This conjecture had been verified via the
agglomeration phenomenon in asphalt binder was more obvious, and simulation results of ref. [98]. The simulation results showed that

7
J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 4. (a, b) are the metallurgical microscope test result of the normal group and the optimal group. Reproduced with permission from ref. [97], Copyright 2019,
MDPI. (c ~ f) are the 3D/2D characterization result of GMA. Reproduced with permission from ref. [101], Copyright 2020, Elsevier. (g) is the SEM result of exfoliated
graphite extracted from hot asphalt. (h) is the SEM result of graphene. (i) is the simulation of the cross-link morphology between asphaltene and graphene.
Reproduced with permission from ref. [102], Copyright 2019, CNKI. (j) is the contact angle of PAN, D-PAN, GNPs/D-PAN with asphalt and water, respectively.
Reproduced with permission from ref. [100], Copyright 2019, Elsevier. (k) is the AFM result of base asphalt and GMA. Reproduced with permission from ref. [103],
Copyright 2021, Elsevier.

among the four components of asphalt, the adsorption of asphaltene and explanation of the mechanism was in the hypothesis stage, and further
graphene was the largest. The authors thought that the dispersion effect research and verification were still needed.
of graphene may be affected by the inter-layer distance of graphene in According to Fig. 4 (j), Z. Su, et al. [100] reported that graphene
asphalt binder. According to the above literature, surfactant can in­ could modify the properties of fiber. Through the contact angle test, it
crease the distance between graphene layers, so can asphaltene. The was shown that the addition of graphene can effectively increase the
reason for the formation of graphene-like substances produced by lipophilicity and hydrophobicity of the composite, which was conducive
expanded graphite after the action of hot asphalt was that asphaltene to the modification of asphalt via using the composite, and the reason for
inserted into expanded graphite and increased the van der Waals force improving the water loss resistance of asphalt binder was also revealed.
between layers. When the asphalt was washed out, the inter-layer dis­ It can be seen that graphene can not only modify asphalt alone, but also
tance between the expanded graphite did not change greatly due to the modify asphalt with other materials, and enhance the effect of other
stability of van der Waals force. It was found that the morphology of materials. X. Li, et al. [103] introduced the diffusion theory and “bee
expanded graphite after washing was similar to that of graphene, which structure” to explain the rheological properties of GMA. It was consid­
also indicated that asphaltene had the intercalation mechanism. The ered that the viscosity of asphalt binder affected the migration velocity
addition of surfactant increased the distance between graphene layers, and resistance of particles. The smaller the viscosity is, the higher the
and was more conducive to the intercalation of asphaltene, thus migration velocity and the smaller the migration resistance of the par­
improving the dispersion effect of graphene in asphalt binder. The ticles are, and the “bee structure” formed by the particles is larger in size

8
J. He et al. Construction and Building Materials 330 (2022) 127222

but less in number. Therefore, according to Fig. 4 (k), the “bee structure” 5.2. Influence of GNPs
of GMA was more and smaller, which meant that the addition of gra­
phene made the viscosity of the base asphalt larger, and the essence of 5.2.1. Macro influence
the change of the “bee structure” was that graphene increased the par­ GNPs are made of flake graphene, and their morphology and struc­
ticle migration resistance and reduced its migration speed in the asphalt ture are very similar to the thin wall of carbon nanotubes. Their thick­
medium. It was also considered that graphene, like asphaltene, can play ness is generally 6–8 nm, bulk density is 0.03–0.1 g/cm3, oxygen content
a role of micelle binding and hinder particle migration. is less than 1%, and carbon content is 99.5%. Due to their unique size
In conclusion, both macro performance test and micro simulation and morphology, they have better mechanical properties in graphene
verification could prove that graphene could effectively improve the and its derivatives. Table 3 summarizes a series of studies on GNPs used
high-temperature performance of asphalt binder. In addition, graphene in modified asphalt in recent years.
could also reduce the emission of asphalt smoke and improve the aging According to the relevant literature in Table 3, M. Han, et al. [107]
resistance and the thermal conductivity of asphalt binder. However, reported that polystyrene (PS) was grafted onto GNPs via in-situ poly­
there were some disputes on the influence of low-temperature perfor­ merization method, and GNPs could be functionalized to change their
mance of asphalt binder. The interaction between graphene and aro­ dispersion in asphalt. The results showed that GNPs can improve the
matic hydrocarbon/asphaltene in the four components of asphalt binder viscoelastic properties of SBS modified asphalt due to the increase of
was stronger than that between graphene and colloid/saturate, which storage modulus and loss modulus; and improve its high temperature
provided a basis for mechanism analysis of GMA. And then, whether stability, due to the increase of softening point, anti-rutting factor, creep
there was interface interaction between graphene and aggregate surface recovery rate of 0.1 kPa and 3.2 kPa, and the decrease of non-
in GMA mixture needed to be further studied. recoverable compliance of 0.1 kPa and 3.2 kPa; and improve its low
temperature performance, due to the decreased of creep stiffness and the

Table 3
Summary of literature on the effect of GNPs on matrix asphalt.
Binder GNPs Effect of GNPs Other findings Ref.
type dosage/%
Penetration Softening Ductility Rutting Recovery Stiffness m
point factor rate modulus value

AH-70 + 0.02, 0.03, PS could be grafted onto GNPs to increase [107]

SBS 0.035, 0.04 its dispersion. The optimum content of
PS-GNPs and GNPs were 0.02 and 0.05 wt
%, respectively.
PG 58–22 2, 4 – – – GNPs could improve water damage [108]
resistance, skied resistance and asphalt-
aggregate adhesive strength. The
optimum content of GNPs was 4%.
PG 58–28 3, 6 – – – – GNPs could increase the work-ability of [109116]
asphalt mixture and reduce the roughness
of aggregate surface texture.
AH-70 + 0.04, 0.05, – – ODA could be grafted onto GNPs to [110]
SBS 0.06, 0.07, increase its dispersion. The optimum
0.08 content of ODA-GNPs was 0.08 wt%
AH-70 + 0.02, 0.04 PS and ODA could improve the fatigue [111]
SBS (PS) life of asphalt. The high temperature
0.04, 0.08 stability and water stability of asphalt
(ODA) mixture based on PS and ODA were
improved.
AH-70 + 0.03, 0.06, – – – GNPs could be coat with PMMA to [112]
SBS 0.09, 0.12 increase its dispersion. PMMA-GNPs
could reduce stress sensitivity of asphalt.
The optimum content of PMMA-GNPs
was 0.06 wt%.
SK-70 + 0.05 – – – GNPs reduced the segregation of rubber [113]
rubber in rubber modified asphalt. There were
powder weak chemical reactions in this process.
AH-70 + 0.02, 0.03, – – – – PS and ODA could improve the aging [114]
SBS 0.035, 0.04 resistance and deformation resistance of
(PS) asphalt. PS-GNPs and ODA-GNPs could
0.04, 0.05, – – – – slow down the high temperature
0.06, 0.07, degradation of SBS polymer and increase
0.08(ODA) their degree of internal cross-linking.
PG 52–34 3, 6 – – – – GNPs could improve the flexural strength [115]
– of asphalt mixture and reduce the
PG 64–34 3, 6 – – – compaction work of asphalt mixture,
+ SBS which is more effective than SBS
modifier. The addition of GNPs has no
effect on the maximum rutting depth. The
stiffness modulus was discrete.
PG 64–22 1, 1.5, 2 – – – The optimum content and mixing time of [117]
GNPs were 2 wt% and 6 min,
respectively. The stiffness modulus was
discrete.
SK-70 0.5, 1, 1.5, 2 – – – GNPs could improve the thermal [118]
diffusivity and thermal conductivity of
base asphalt.

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J. He et al. Construction and Building Materials 330 (2022) 127222

increased of ductility at 5 ◦ C and creep rate m value; and improve its Interestingly, M. Hafeez, et al. [108] thought GNPs had good dispersion
fatigue resistance, the decrease of damage rate. Moreover, it was found in itself, and did not need to be functionalized to increase its dispersion,
that the optimum content of GNPs was 0.05%, while that of PS-GNPs which was not consistent with ref. [107,110,112], so as to save the
was 0.02%, which was based on the quality of SBS modified asphalt. preparation cost. It was found that GNPs could improve the high tem­
M. Han, et al. [110], continued to use the same method, selected octa­ perature stability of base asphalt, via the increase of softening point,
decylamine (ODA) to graft onto GNPs, drew a conclusion similar to anti-rutting factor and the decrease of phase angle; and improve the
[107], that is, ODA-GNPs can improve the viscoelastic properties and permanent deformation resistance via the decrease of the rut depth; and
high temperature stability of SBS modified asphalt, and ODA can reduce the the water sensitivity via the increase of the coating ratio of
improve the dispersion of GNPs in asphalt binder, the optimum content asphalt on the aggregate surface (increase up to 70%); and improve the
of ODA-GNPs was 0.08%, based on the quality of SBS modified asphalt. pull-off tensile strength via the increase of the adhesion of asphalt (in­
However, it did not carry out a detailed test on the low temperature crease up to 56%); and anti-sliding performance via the increase of the
performance. However, the optimal dosage of ODA-GNPs obtained was British Pendulum Number parameter (increase up to 83%). The opti­
the highest dosage of the designed experimental dosage, which could mum content of GNPs was 4%, which was different from the results of
not fully explain the optimal dosage of ODA-GNPs, that was, the optimal ref. [107].
dosage may be greater than 0.08%. Besides, the dosage optimization L. P. Ingrassia, et al. [109] found that the addition of GNPs reduced
curve was not made to determine the optimal dosage. Moreover, when the required for compaction work of asphalt mixture. Based on the
the content of ODA-GNPs was 0.08%, its anti-rutting factor was less than Newton state, the relationship between asphalt viscosity and aggregate
that of SBS modified asphalt, so its role in improving high temperature friction was established via simulating the compaction conditions and
performance had some fluctuations, which needed further study. PS and tribological characteristics of aggregate. However, it was considered
ODA were added to functionalize GNPs respectively, and the optimal that under the conventional mixing conditions, asphalt could not be
content of GNPs decreased (less than 0.05%), while ODA increased Newtonian state, and the aggregate could not be completely free. The
(more than 0.05%). It can be seen that different functional materials friction factor formed by compaction was inevitably affected by the
have different modification effects on GNPs. L. Ji, et al. [111] reported surface roughness of aggregate. Because the base surface of simulated
that PS and ODA were selected as GNPs surface functional materials. It aggregate surface texture is smooth plane, it cannot simulate aggregate
was considered that PS-GNPs and ODA-GNPs could significantly surface texture completely. Therefore, T. Yan, et al. [116] processed the
improve the elastic properties and viscosity of SBS modified asphalt, surface texture of simulated aggregate, so that it could accurately and
reduce the sensitivity of its elasticity and viscosity to temperature and effectively simulate the real situation of aggregate surface. Using the
frequency, and significantly improve its creep recovery rate of 0.1 kPa same method, it was found that the reason of changing the workability
and 3.2 kPa, with the increase rate up to 112.55%, and significantly of asphalt mixture was not caused via the change of asphalt viscosity by
improve its fatigue life, with the increase rate up to 272.79%. However, GNPs, but via the change of asphalt-aggregate surface roughness by
it was considered that GNPs cannot significantly improve the low tem­ GNPs.
perature performance of asphalt, and the high content of GNPs can Y. Chen, et al. [113] reported that GNPs could effectively improve
reduce the low temperature performance of asphalt to a certain extent. the high temperature stability of rubber asphalt, due to the significant
interestingly, this results here are inconsistent with those of [107,110]. increase of its anti-rutting factor and multi-stress creep recovery rate;
Both the water stability and high temperature permanent deformation and also improve the low temperature stability due to the decrease of the
resistance of asphalt mixture based on PS-GNPs and ODA-GNPs were low temperature stiffness modulus and the increase of the m value. It
improved. Through performance analysis and comparison, it was was also found that GNPs could effectively improve the segregation of
considered that the modification effect of 0.02% PS-GNPs and 0.08% rubber in asphalt, which was conducive to the adhesion between
ODA-GNPs was the best, and the modification effect of 0.02% PS-GNPs modified asphalt and aggregate. J. Le, et al. [115] considered that the
was better than that of 0.08% ODA-GNPs. Y. Wei et al. [114], and then addition of GNPs can improve the low-temperature flexural strength of
continued to select PS-GNPs and ODA-GNPs for short- and long-term asphalt materials (up to 1 time), and can effectively reduce the
aging analysis. It was found that the viscoelastic properties and soft­ compaction work of asphalt mixture, that is, when the target void ratio
ening point of the modified asphalt increased significantly after short- of asphalt mixture was reached, the number of rotary compaction was
and long-term aging, and the complex shear modulus and deformation reduced by 20 ~ 40%. However, the addition of GNPs had no significant
resistance of the modified asphalt increased significantly after long-term effect on the low temperature relaxation property and the creep stiffness
aging. Thus, it was considered that GNPs could improve the anti-aging of the asphalt binder. It was also pointed out that there was an optimal
ability of asphalt. Moreover, it is found that the ductility of ODA- GNPs content, but the specific content was not clearly pointed out or
GNMA decreased obviously when the content of ODA-GNPs was more calculated. It was believed that the reduction of compaction work may
than 0.05%. It was considered that the possible reason was that after the be due to the lubrication of GNPs, but it was not characterized and
dosage was more than 0.05%, ODA-GNPs occurred agglomeration analyzed here, and it was not clear how it affected the strength of binder
phenomenon to cause uneven dispersion, resulting in poor compatibility aggregate interface. H. Brcic [117] thought that the addition of GNPs
with asphalt. Interestingly, in ref. [111], it was pointed out that the improved the permanent deformation resistance of asphalt, but at the
optimal dosage of ODA-GNPs was 0.08%. However, in ref. [114], it was same time made it easier to crack at low temperature. X. Jia, et al. [118]
considered that serious uneven dispersion will occur when the dosage believed that GNPs could improve the stability of base asphalt at high
exceeded 0.05%. Therefore, further research is needed for this specific temperature, but because of the agglomeration phenomenon of GNPs, it
dosage. hindered the mobility of asphalt molecular chain at low temperature,
L. Ji, et al. [112] reported that PMMA was coated on GNPs surface and causes local stress concentration, which affected its low temperature
via microwave polymerization method to increase its uniformity and performance. GNPs can also effectively improve the thermal conduc­
dispersion in asphalt binder, and its optimum content was 0.06%. It was tivity and thermal diffusivity of base asphalt.
found that the elastic modulus (14.2%) and creep recovery rates (76% According to the above literature, GNPs can improve the high tem­
and 350%) of 0.1 kPa and 3.2 kPa were increased via adding the optimal perature performance of asphalt, which is manifested in the improve­
PMMA-GNPs content, and the stress sensitivity of PMMA-GNMA could ment of softening point, anti-rutting factor and corresponding multi-
be decreased. However, the effect of modification decreased sharply stress creep recovery rate of modified asphalt, and the reduction of
when the dosage was higher than that. It was considered that excessive multi-stress non-recoverable compliance. However, there are different
PMMA-GNPs would increase the inter-molecular force of itself, caused opinions on the effect of GNPs on the low-temperature performance of
agglomeration phenomenon and reduced the modification effect. asphalt. Some literature show that the low-temperature performance is

10
J. He et al. Construction and Building Materials 330 (2022) 127222

improved, whereas the others show that the low-temperature perfor­ 5.3. Influence of GO
mance is impaired. The difference in opinions may be due to the use of
surfactant and the specific dosage. Moreover, there are many contra­ 5.3.1. Macro influence
dictions in the optimal content on GNPs. The optimum content varies GO is similar to graphene and GNPs, but it has rich oxygen-
vastly from 0.02% to 2%, which has not been accurately determined. containing functional groups. It is because of the introduction of
oxygen-containing functional groups that their properties are diversi­
5.2.2. Micro influence fied, which have both hydrophilicity and hydrophobicity. The oxygen-
According to the literature, the micro characterization and simula­ containing functional groups of GO are not randomly distributed, but
tion results of GNMA are shown in Fig. 5. highly correlated. At present, it is considered that epoxy resin and hy­
According to Fig. 5 (a-o), PS and ODA had successfully functionalized droxyl are connected on the base surface of the lamina, and carboxyl and
GNPs via in-situ grafting technology, while PS grafting was similar to carbonyl are connected at the edge of the lamina [119–121]. In addition,
wrapping independent GNPs, and this grafting produced only the sur­ GO can be reduced to graphene to restore its highly conjugated struc­
face functional groups, did not embedded into the layers of GNPs, which ture. Table 4 summarizes a series of studies on GO used in modified
meant that the crystal plane distance of GNPs was not affected. In the asphalt in recent years.
process of ODA grafting, not only the surface of GNPs was modified, but According to the relevant literature in Table 4, W. Zeng, et al. [122]
also some branched chains between layers were grafted, and the dis­ believed that GO could improve the high and low temperature perfor­
tance between crystal planes was increased. Both of them improve the mance of base asphalt, based on the change of complex modulus at high
lipophilicity and compatibility of GNPs, which is beneficial to the and low temperature. It was considered that the addition of 1% GO is
modification of asphalt. However, compared with PS grafting, ODA is better than 3%. It was found that the effect of GO on asphalt aging-
more irregular and sequenced. Fig. 5 (p, q) shows the basic principle of resistance is not obvious via RTFOT and PAV test. Meanwhile, when
water damage resistance of asphalt mixture based on PS-GNPs and ODA- GOMA is heated to about 115 ◦ C, it would release a lot of carbon dioxide,
GNPs. In the process of preparing modified asphalt, the functional which also provided a certain reference for the research and develop­
groups on the surface of GNPs and SBS modifier expand into long chains ment of flame retardant asphalt. S. Wu, et al. [123] suggested that GO
under low-speed stirring and static conditions, and then form a spring- could improve the fatigue cracking resistance of SBS modified asphalt.
like network structure. The lipophilicity of GNPs surface molecules By analyzing the C– – O and S–– O functional group change index, vis­
also plays a key role in the exclusion of water molecules, which further cosity aging index (VAI), residual penetration ratio (PRR), softening
improves the ability of GNPs to resist water damage. The water damage point increment (SPI) and residual ductility ratio (DRR), it was found
resistance of PS-GNMA is better than that of ODA-GNMA. Meanwhile, it that GO could effectively improve the heat-oxygen aging resistance of
was also found that PS reduced the optimal content of GNPs, while ODA SBS modified asphalt. It was considered that the complex modulus of
increased it. Therefore, it is suggested that the changes of GNPs content asphalt decreases with the addition of GO, and the content of 3% was
and lipophilic or hydrophilic properties may be related to the modifi­ better than that of 1%. Interestingly, there is a contradiction between
cation effect, arrangement order and crystal plane distance of functional this part of the conclusion and the ref. [122]. The main difference is that
groups in the functionalization treatment, which still needs further ref. [122] used RTFOT and PAV for aging, while ref. [123] used UV and
research and demonstration. Moreover, whether the water stability is RTFOT for aging, which still needs further research and verification. R.
caused by the introduction of functional groups and lipophilicity is not Wang, et al. [137] adopted the same research method described by ref.
caused by GNPs are still not clear. [123]. The effect of GO on the aging resistance of matrix asphalt was
In Fig. 5 (t, u), it can be seen that the texture characteristics of the studied. It was found that GO could effectively improve the short-term
aggregate surface of the base asphalt and GNMA mixture. M. Hafeez and long-term aging of base asphalt. However, it is different from the
et al. [108] thought that GNPs improve the skid resistance and polishing conclusion of ref. [123] that the optimal content of GO is 1.5%. It is
resistance, and increase the friction of GNPs asphalt pavement. More­ considered that the difference of dosage may be the influence of SBS
over, it is observed that the surface of the aggregate coated with matrix modifier. D. Singh, et al. [135] studied the effects of GO on the chemical
asphalt is smoother, while the surface of the aggregate coated with GNPs composition, rheological properties and micro-structure of asphalt
modified asphalt is coarser, which confirms that the improvement of the binder. It was considered that the addition of GO increased the viscosity
anti-sliding ability is caused by the increase of the surface roughness of of asphalt binder, resulting in the increase of mixing temperature and
the aggregate by GNPs. L. P. Ingrassia et al.[109] thought that GNPs compaction temperature. Although it had a positive effect on the high
could increase the rough texture of smooth asphalt surface, as shown in temperature performance and fatigue life of asphalt, its optimal dosage
Fig. 5 (x, y). The addition of GNPs in modified asphalt makes it easier to is not consistent. 1% of GO had the best effect on high temperature
embed GNPs into aggregate texture, as shown in Fig. 5 (v, w). Because of rutting performance, and 2% of GO had the best effect on fatigue life and
the large specific surface area of GNPs, the interfacial adhesion between bond yield energy. This view is similar to the conclusion of ref. [134].
asphalt and aggregate was also increased. The assumption of rough Meanwhile, it was found that the nitrogen element decreased signifi­
texture on asphalt surface is in consistent with that in ref. [108]. How­ cantly after adding GO via the element analysis. Therefore, it was
ever, as shown in Fig. 5 (R, s), the surface of rubber asphalt is rough and speculated that there were NO2 and CO2 emissions in the process of
has a strong sense of particles in the local uplift. After adding GNPs into high-temperature preparation of modified asphalt, which is similar to
rubber modified asphalt, the surface is smooth and has no sense of the relevant conclusion of ref. [122].
particles. Y. Chen et al. [113] thought that the addition of GNPs could K. Liu, et al. [124] considered that GO could improve the viscosity,
make the rubber powder evenly and compactly dispersed in the base anti-rutting factor and multi-stress creep recovery rate of base asphalt
asphalt, forming a stable system, but the mechanism was not explained. and SBS modified asphalt. However, the effect of improving the low-
So, according to the characterization results of modified asphalt in ref. temperature crack resistance is not very obvious. It was found that the
[113], it does not show rough surface, which is quite different from the glass transition temperature Tg did not change before and after adding
relevant conclusions in ref. [108,109]. A possible explanation of this is GO via DSC test, which meant that GO had little effect on the low-
that GNPs did not make the rubber particles evenly dispersed, but GNPs temperature performance of asphalt binder. It was also found that the
were filled into the rough texture of the surface of the rubber particles, content of GO should not exceed 0.2%, based on the amount of asphalt
making them smooth and silky, which needed to be further binder. It is worth noting that there are chemical reaction and physical
demonstrated. reaction blending in base asphalt system, but there was only physical
reaction in SBS modified asphalt system via FTIR test. Which was also
different from the above research on graphene and GNPs. Meanwhile,

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J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 5. (a ~ f) are the SEM results of GNPs and PS-GNPs, and (n) is the three-dimensional simulated structure of PS-GNPs, Reproduced with permission from ref.
[107], Copyright 2018, Elsevier. (h ~ m) are the SEM results of GNPs and ODA-GNPs, and (o) is the three-dimensional simulated structure of ODA-GNPs, Reproduced
with permission from ref. [110], Copyright 2018, Elsevier. (p, q) are the simulation mechanism of water damage resistance of PS-GNPs and ODA-GNPs. Reproduced
with permission from ref. [114], Copyright 2018, Elsevier. (r, s) are the SEM results of rubber modified asphalt and the rubber-GNPs modified asphalt. Reproduced
with permission from ref. [113], Copyright 2020, Elsevier. (t) is the SEM result of the aggregate coated with base asphalt, and (u) is the SEM result of the aggregate
coated with GNPs modified asphalt. Reproduced with permission from ref. [108], Copyright 2019, MDPI. (v, w) are based on lubrication simulation between ag­
gregates (v without GNPs, w with GNPs), and (x, y) are based on lubrication simulation between asphalt materials (x without GNPs, y with GNPs). Reproduced with
permission from ref. [109], Copyright 2019, ASCE.

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J. He et al. Construction and Building Materials 330 (2022) 127222

Table 4
Summary of literature on the effect of GO on asphalt.
Binder type GO Effect of Graphene Other findings Ref.
dosage/%
Penetration Softening Ductility Rutting Recovery Stiffness m
point factor rate modulus value

70A, 90A 1, 3 – – – – The effect of GO on anti-aging of asphalt [122]

was not obvious. GOMA would release a
lot of CO2 during heating. The content of
1% GO was better than that of 3%.
90A, SBS 1, 3 – – – GO could improve the thermal/oxidative [123]
aging resistance and the fatigue cracking
resistance of asphalt. The content of 3%
GO was better than that of 1%.
PG 64–22, 0.02, 0.05, – – – The effect of GO on the cracking [124]
PG 0.1, 0.2, 1 resistance of asphalt was not obvious.
58–34 + The optimum content of GO for base
SBS asphalt and SBS modified asphalt were
0.05% and 0.2%.
PG 64–22 0.05 – – – The mixing and compaction temperature [125126]
+ Sasobit of asphalt mixture could be reduced via
PG 64–22 0.05 – – – using GO + WCO or Sasobit. The addition
+ WCO order of modifier should be GO first, and
then warm mix additives.
AH-70 + 0.05 – – The addition of warm mix additives [127]
WCO/ could improve the mechanical strength
Sasobit and low temperature crack resistance of
GOMA.
SK-70# + 0.5, 1, 1.5, – – GO was modified via bromobutane and [128]
SBS 2, 2.5, 3 SBS to synthesize a new modifier. The
asphalt modified via the new modifier
showed no obvious segregation.
SK-90# + – GO could improve the water stability of [129]
rubber rubber asphalt mixture.
powder
60/70 0.5, 1, 1.5, – – – – The optimum content of GO was 2%. GO [130]
2, 2.5 could improve the resilient modulus, the
permanent deformation and the moisture
stability of HMA mixture.
AH-70 0.006, – – The aromatics were easily converted into [131]
0.012, resins in the GOMA. GO had little effect
0.024, on the adhesion of base asphalt.
0.048
70A 0.1, 0.3, – – – – The optimum content of GO was [132]
0.5, 0.7, 0.5–0.7%. The bonding of resin/GO was
0.9 the most stable, followed by aromatic/
GO, and saturate/GO was the weakest.
SK-70# + 0.2, 0.3, – – The optimum content of new modifier [133]
SBS 0.4, 0.5, was 0.02%. GO could be modified via
0.6 thiolene click reaction to synthesis new
modifier.
50/70 + 0.1, 0.2, – – – – The optimum content of CR was 9.8%, [134]
crumb 0.3, 0.5 but that of GO was uncertain. The
rubber composite effect of GO and CR was better
for HMA.
AC30 1, 2, 3 – – – – – GO could improve the viscosity, fatigue [135]
life and yield energy of asphalt. The
optimum content of GO was uncertain.
60/70 0.5, 1, 1.5, – – – – The content of GO had an important [136]
2, 2.5 effect on the volume parameter of the
mixture. The optimum content of GO and
asphalt were 1.8 and 5.3% for the mix
type AC-10.
70A 0.5, 1, 1.5 – – – GO could improve the short- and long- [137]
term aging of asphalt. The optimum
content of GO was 1.5%.

the research team also studied GO warm mix asphalt mixture. The temperature crack resistance was significantly improved. So it is
composite modification of GO with 3% Sasobit and 5% waste cooking oil thought that 3% Sasobit-GO composite modified asphalt was suitable for
(WCO) was studied and analyzed [125], and then the addition sequence high-temperature areas, and 5% WCO-GO composite modified asphalt
of GO and warm mixing agent was studied and analyzed [126]. It was was suitable for low-temperature areas. Through the study of modifier
found that the viscosity, mixing temperature and compaction tempera­ addition sequence, it was found that the best composite modification
ture of GOMA were decreased significantly after adding warm mix effect is to add GO first, followed by warm mixing agent. J. Zhu, et al.
agent, and the reduction of maximum temperature was 17 ◦ C. Inter­ [127] reported the comprehensive analysis of the pavement perfor­
estingly, it was also found that after adding Sasobit, its high-temperature mance of GO-hot/warm mix asphalt mixture based on the above
performance was significantly improved; after adding WCO, its low- research results. It was found that the resistance to water stability, high

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J. He et al. Construction and Building Materials 330 (2022) 127222

temperature stability, low temperature cracking resistance, aging asphalt and the disappearance of C– – C bond stretching vibration in base
resistance and compression resilience modulus of GOMA mixture could asphalt. The research team also optimized the content of GO via
be all improved correspondingly, but the WCO reduced the cohesion of modeling and optimization [136]. Based on the analysis of variance, the
the asphalt molecule. During the aging process, the unsaturated fatty research team believed that the content of GO directly affected the
acids of WCO could be also easily volatilized, resulting in the decrease of volume parameters of asphalt mixture, which could directly affect the
water resistance and aging resistance of GOMA mixture. Sasobit could road performance of asphalt mixture [140–144]. And it was considered
increase the stiffness of asphalt and reduce its low temperature crack that the optimum content of GO and asphalt were 1.8% and 5.3%,
resistance. It is believed that there are obvious differences in the com­ respectively. It is reckoned that these conclusions reflect the influence of
posite effect between warm mix agent and GO, and the main reason may GO on the adhesion of aggregate, but the above ref. has made relevant
be that the oxygen-containing functional groups in GO reacted with elaboration based on its results, and has not studied its effect mecha­
warm mix agent, resulting in different modification effects. nism, which still needs further research and exploration.
S. Duan, et al. [128] reported that in order to solve the problems of R. Yu, et al. [131] considered that although GO had a certain influ­
compatibility and agglomeration phenomenon, bromobutane and SBS ence on the penetration, softening point and ductility of base asphalt,
modifier were used to modify GO. The butyl functional group and SBS and the influence range was very small and almost negligible, but it has a
modifier were grafted into GO, and the butyl functional group was used significant improvement on the low temperature crack resistance of
to improve the lipophilicity of GO, so as to improve the above problems. asphalt binder. Through the research and analysis of the influence of GO
It was believed that the successful grafting of -C4H9 onto GO surface can on the four components of base asphalt, it was considered that the ar­
be stabilized by the stacking of π - π bonds from SBS. It was found that omatic component was easy to be converted into resin in GOMA system,
the new modifier can significantly improve the softening point, ductility that is, this system was prone to happen aging phenomenon. The authors
and multi-stress recovery rate of base asphalt, and the optimal dosage of think that the initial addition of GO is only 0.006%, which does not show
the new modifier was 1%. It is noteworthy that the effect of GO on the the effect of GO. Moreover, G. Huang, et al. [145] reported that when
phase angle of asphalt is different from that of graphene and GNPs. With high temperature shearing was used in the preparation process, it was
the increase of temperature, the phase angle first decreases and then easy to cause asphalt aging phenomenon, especially after adding
increases, and a turning point appears at about 60 ◦ C. J. Li, et al. [133] nanomaterials, and the aging phenomenon of modified asphalt was
reported the modification of SBS modified asphalt via using GO modi­ particularly serious. So, the above phenomenon was appeared. It is not
fied by 3-mercaptopropyltriethoxysilane. It was believed that the -SH on difficult to find that when the content of GO reaches 0.048, the aro­
the modified GO was conducive to the reaction with SBS molecular matics of GOMA do not turn into resin. At the same time, it was also
chain, which was also conducive to the uniform dispersion of GO in considered that GO had no obvious effect on the viscosity of asphalt,
asphalt binder. Meanwhile, the modifier could also improve the high which contradicted the findings in ref. [124,132]. Moreover, there was
temperature performance of SBS modified asphalt, and the optimal no chemical reaction between the two, only physical adsorption, which
content was only 0.02%. It is considered that GO can be modified by was different from the conclusion in ref. [130]. Q. Zeng, et al. [132]
some compounds. The oxygen-containing functional groups of GO can reported that the influence of GO on the three major indexes of asphalt
be replaced by other functional groups, so as to play the role of func­ was consistent with ref. [127,130] and the relationship model between
tional groups after replacement, and enrich the performance charac­ GO and SARA was established. It was considered that the interaction of
teristics of GO, which provides a certain reference for the further GO-resin was the strongest, followed by GO-aromatic, and the GO-
development of multifunctional GO. Moreover, it can be found from ref. saturate was the weakest, which was obtained by density universal
[128,133] that the optimal amount of modified GO in SBS modified function theory. It was also considered that GO only reacted with
asphalt is quite different from that of unmodified GO, which also reflects hydrogen atoms on SARA branch chain to form stable hydrogen bond,
the role of functional groups replacement. but did not produce other reactions, which was contrary to the conclu­
M. Lin, et al. [129] reported the modification of rubber asphalt with sion in ref. [130]. Meanwhile, because of their benzene ring-like struc­
GO. SEM results showed that GO could form the denser and more stable ture, GO was easy to stack with resin or asphaltene. When the inter-layer
network structure with rubber powder. And GO could significantly distance was increased, the crystallization phenomenon was decreased,
improve the high temperature and low temperature performance of which was similar to the description of graphene in ref. [102]. There­
rubber asphalt, as well as the dynamic stability, low temperature crack fore, the authors think that the similar graphene-like materials may have
resistance and water stability of the corresponding asphalt mixture. the similar properties. It is worth noting that according to the simulation
However, the specific content and preparation process of GO were not results, GO can effectively inhibit the volatilization of saturated com­
described in detail, and the related research still needed to be deepened. ponents, thus improving the aging resistance of asphalt binder, which is
B. B. Singh, et al. [134] reported the composite modification of base in contradiction with the conclusion in ref. [131].
asphalt with GO and rubber powder produced by waste tires. It was In addition to the relevant research results summarized in Table 4, R.
found that the optimal content of waste rubber powder was 9.8%, but Wang, et al. [138] studied the effects of GO on the long-term and short-
the optimal content of GO could not be determined. The reason was that term aging of asphalt binder, based on thermodynamic parameters and
low content of GO improved Marshall stability greatly of asphalt internal healing properties. It was found that with the increase of GO
mixture, while high content of GO improved tensile strength and content, the surface free energy and internal healing performance of
freeze–thaw splitting strength greatly. Moreover, it was found that there asphalt were improved, that was, the cohesion of asphalt binder and the
was a partial chemical reaction between GO and waste rubber powder adhesion of asphalt-aggregate are improved. Short term aging has a
via FTIR test, which made it more closely combined. These conclusions positive effect on the surface free energy and internal healing perfor­
are consistent with the relevant description in ref. [129]. mance of asphalt, but long-term aging has a negative effect on it.
A.M. Adnan, et al. [130] reported that the optimum content of GO Similarly, J. Zhu, et al. [139] reported that the adhesion of GOMA-
was 2%. Then the road performance of graphene GOMA mixture was aggregate was studied via using the research method similar to that in
studied in detail. It was considered that GO can significantly improve the ref. [138], and AFM test was added to further prove it, which also found
resilient modulus (increased by 55%), immersion Marshall stability the conclusion similar to that in ref. [138]. It was considered that the
(increased by 10%), freeze–thaw splitting strength (increased by alkalinity of aggregate would directly affect the adhesion of asphalt-
14.54%) and flexural strength (increased by 117.2%) of asphalt mixture, aggregate. The adhesion between aggregate and limestone was the
and reduce its permanent deformation (decreased by 64.47%). Mean­ highest, followed by basalt and granite. Moreover, GO was beneficial to
while, it was also considered that there was the chemical reaction be­ slow down the effect of aging on the decrease of interfacial adhesion of
tween GO and asphalt, due to the formation of C-Cl bond in modified asphalt-aggregate, and SBS modifier and GO could be used to prepare

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J. He et al. Construction and Building Materials 330 (2022) 127222

high viscosity asphalt for OGFC pavement. and simulation results of GOMA are shown in Fig. 6 ~ 9.
According to Fig. 6 (a), the preparation of GOMA by W. Zeng, et al.
5.3.2. Micro influence [122] is shown. It was found that when GOMA was heated to 115 ◦ C, its
Unlike graphene and GNPs, the interaction between GO and asphalt volume would expand rapidly, which was three times of that at room
binder is more complex due to the influence of oxygen-containing temperature. At the same time, it had been proved that the gas was CO2,
functional groups on the interface of GO. There are great differences and its volume would return to normal after cooling to room tempera­
on whether there are chemical reactions in this GOMA system among ture. The authors thought that the ref. [122] does not clearly indicate the
related researchers. Via FTIR test, some researchers thought that there go content, so it is impossible to accurately infer whether the boiling
was chemical reaction and physical reaction between GO and asphalt, reaction phenomenon is caused by the GO content reaching a certain
but some thought that there was only physical reaction but no chemical critical point, or whether the phenomenon can also be caused by a small
reaction. In this paper, the results of FTIR tests in the above references amount of GO. But, it is clear that GO and asphalt have CO2 generation
are summarized, and the results are shown in Table 7. at high temperature. It is worth further studying whether the carbon
According to Table 7, ref. [124,128,133] believed that when the GO element is provided by GO or asphalt, which is helpful to reveal the
and SBS modifier were modified asphalt simultaneously, there was no internal meaning of the reaction between them. Fig. 6 (b, c) shows the
chemical reaction in the system, but only physical reaction. Meanwhile, micro-structure of rubber asphalt and the rubber asphalt added by GO,
it also thought that GO have strong adsorption with SBS modifier or the respectively. M. Lin, et al. [129] thought that the phenomenon of rubber
chain reaction with its molecular group, which will promote its uniform particles wrapped by asphalt could be clearly observed in Fig. 6 (b).
dispersion in asphalt medium and form a stable network structure, However, when GO was added, it was found that the wrapping phe­
without chemical reaction with substances in asphalt binder. Similarly, nomenon could not be observed obviously, and the phenomenon
ref. [131,132,135,137] also found that there was no chemical reaction developed to the mutual blending of the two. Thus, it was considered
between GO and asphalt, only physical adsorption. Different from the that GO was beneficial to the bonding between rubber particles and
above, this part did not add any additives, that was, the interference of asphalt. Similarly, B. B. Singh, et al. [134] reported that it was obvious
additives was eliminated. It was believed that although the new func­ from Fig. 6 (d, e, f) that when GO was added into rubber asphalt, the
tional group could be produced in asphalt binder, the functional group roughness of rubber particles in asphalt was obviously improved, but the
may be the superposition effect of the two, which did not mean that the presence of GO was also observed obviously. The authors believe that
two had a chemical reaction. Interestingly, there was no additive to be there are two reasons why GO can improve the compatibility of rubber
added in ref. [124,125,130], which was considered that chemical re­ particles in asphalt binder. One is that GO reacts with rubber to form a
action occurred in GOMA system, that is, the generation of functional new compound modifier, and the other is that GO improves the bonding
groups OH, C– – O, C–H and C-Cl, and the disappearance of functional properties of asphalt, so as to improve their compatibility. However,
group C≡C. Obviously, there is a contradiction between the two views. according to Fig. 6 (f), the existence of GO can be clearly observed, so the
The authors thought that the functional group O–H may be generated by authors reckon that the latter reason is more likely.
the GO in GOMA system, but the changes of other functional groups are According to Fig. 7 (a-1 ~ a-4), Q. Zeng, et al. [132] considered that
still the effective evidence of this conclusion, and further research is GO was the dispersed phase in GOMA system, while asphalt was the
needed to verify this problem. dispersion medium, and GO was wrapped by asphalt and uniformly
In ref. [125,126,134], when additives Sasobit, WCO and CR were dispersed in the dispersion medium. The van der Waals force between
added, it was considered that there were both chemical and physical GO molecules was reduced due to the effect of oxygen-containing
reactions in the system. Moreover, the lost functional group of GO was functional groups of GO, and it was easy to disperse uniformly in the
O–H, which indicated that the functional group was easy to react or case of small amount of GO. However, with the increase of the content of
replaced with other groups. The authors believe that the description of GO, the interaction between GO molecules was increased, which
chemical reaction in the system mentioned above was relatively simple. reduced the dispersion of GO molecules in asphalt binder and led to the
There are three possibilities as follows: In the first case, the additives agglomeration phenomenon of GO molecules. According to Fig. 7 (b-1
react with GO, such as the replacement of functional groups, but do not ~ b-4) and Fig. 7 (c-1 ~ c-4), this phenomenon could also be clearly
react with asphalt; In the second case, additives act as a special catalyst, observed in the studies of D. Singh, et al. [135] and A. M. Adnan, et al.
which make GO react with asphalt; In the last case, additives, GO and [136], that was, when the GO content gradually increased, it would
asphalt participate in the chemical reaction, which still need further appear obvious agglomeration phenomenon. In ref. [136], it was also
research and verification. considered that the sizes of GO agglomerates were usually 5 μm in
According to the existing literature, the relevant characterization asphalt binder. The authors reckon that the morphology of GO in asphalt

Table 7
Summary of literature on FTIR test of GOMA.
1
Ref. Chemical reaction Physical reaction additives Types of additives Wavenumber/cm− Change of functional groups

[124] √ √ × – 3433.78, 1643.65, 887.80/861.16 O–H, C––O, C–H (+)

× √ √ SBS – –
[125] √ √ × – 3436.92 O–H (+)
√ √ √ Sasobit 1140.62, 1539.54, 669.22/1339.43; 3436.92 C-O, C–
–C, C–H (+); O–H(-)
√ √ √ WCO 1140.62, 1539.54, 669.22/1339.43, 1747.77; 3436.92 –C, C–H, C–
C-O, C– –O (+); O–H (-)
[126] √ √ √ Sasobit 1140.30,1907.16; 3436.92 C-O, C–
–O (+); O–H (-)
√ √ √ WCO 669.22, 1139.52, 1747.20; 3436.92 C–H, C-O,C––O (+); O–H (-)
[128] × √ √ SBS + C4H9Br – –
[130] √ √ × – 611.00, 2186.00 C-Cl (+); C≡C (-)
[131] × √ × – – –
[132] × √ × – – –
[133] × √ √ SBS + KH580 – –
[134] √ √ √ CR 2921.00, 2841.00; 3410.00 CH3–, CH2– (+); O–H (-)
[135] × √ × – – –
[137] × √ × – – –

Notes: (+) indicates the formation of functional groups; (-) indicates the disappearance of functional groups.

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J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 6. (a) is the boiling effect phenomenon of GOMA. Reproduced with permission from ref. [122], Copyright 2017, Mdpi. (b, c) are the micro-structure of RA and
GORA. Reproduced with permission from ref. [129], Copyright 2019, De Gruyter. (d, e, f) are the SEM images of GOMA, CRA and CR-GOMA, respectively.
Reproduced with permission from ref. [134], Copyright 2014, KeAi.

Fig. 7. (a-1/2/3/4) are the SEM images of base asphalt (magnified 1000 times), 0.5%GOMA (magnified 1000 times), 0.5%GOMA (magnified 3000 times) and 0.9%
GOMA (magnified 3000 times), respectively. Reproduced with permission from ref. [132], Copyright 2020, Elsevier. (b-1/2/3/4) are the SEM image of base asphalt,
1%GOMA, 2%GOMA and 3%GOMA, respectively (magnified 25X). Reproduced with permission from ref. [135], Copyright 2020, ASCE. (c-1/2/3/4) are the SEM
image of base asphalt, 1%GOMA, 1.5%GOMA and 2%GOMA, respectively (magnified 10000X). Reproduced with permission from ref. [136], Copyright 2020, Taylor
& Francis Group.

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J. He et al. Construction and Building Materials 330 (2022) 127222

can be clearly observed via SEM images. But in order to determine the complex chemical and physical properties and molecular structure,
specific reaction form, it is necessary to combine FTIR or other charac­ which also provides a reliable basis and conditions for the preparation of
terization methods. According to Fig. 7 (a-2), Fig. 7 (c-2) and Fig. 7 (c-4), modified asphalt with better performance.
it is obvious that the agglomeration phenomenon is not obvious when According to Fig. 9(a ~ c), Q. Zeng, et al. [132] simulated the
the content of GO is less than 0.5%. However, when the content of GO electron density of GO with saturates, aromatics and resins to reflect the
increases from 1% to 2%, the stacking phenomenon between the layers interaction strength between them. Via the comparison of binding en­
of GO can be clearly observed. ergy, it could clearly show that the interaction of GO-resin was the
According to Fig. 8(a ~ d), S. Duan, et al. [128] reported that the strongest, followed by GO-aromatic, and the GO-saturate was the worst.
morphology of GO, compound C4H9-GO, SBS modifier and compound According to Fig. 9(e ~ l), J. Zhu, et al. [139] reported the morphology
C4H9-GO/SBS were observed via SEM image. The process of GO modi­ characteristics of base asphalt, GOMA, SBS modified asphalt and SBS/
fied by group -C4H9 is shown in Fig. 8(e), and the mode of interaction GO modified asphalt before and after PAV aging, via AFM test. It was
between SBS modifier and modified GO is shown in Fig. 8(f). According considered that the addition of GO made the boundary between
to Fig. 8(b), it can be clearly observed that GO is modified by group continuous phase and dispersed phase clearer, and increased the number
grafting. Fig. 8(d) also clearly shows that the SBS modifier and the of the “bee structure”. When GO was added into SBS modified asphalt,
modified GO form a chain reaction, and the molecular chain of SBS the number and size of the “bee structure” were still increased. After
modifier adsorbs with each other to form a dense network structure. PAV aging, it was found that the “bee structure” of asphalt without GO
Similarly, J. Li, et al. [133] showed the simulated morphology of GO was decreased and its size was increased, significantly. However, the
modified by compound KH580 and the interaction between the het­ number and size of the “bee structure” of asphalt with GO did not change
erogeneous GO and SBS modifier via Fig. 8(g, h), respectively. It also greatly, that was, the viscosity of asphalt was changed little and the
showed that the chain reaction occurred, like ref. [128], and the het­ cohesiveness of aggregate was increased. This phenomenon also ex­
erogeneous GO and SBS modifier formed a staggered network structure. plains that the addition of GO makes the durability and aging resistance
Therefore, the authors think that the above literature all show the chain of the asphalt mixture better. This phenomenon was also found in gra­
reaction between the modified GO and SBS modifier, whose effect is not phene in reference [103], so it is considered that materials with
only reflected in increasing the stability of SBS modifier network graphene-like structure can cause the change of the “bee structure” in
structure and its compatibility in asphalt, but also in increasing the road asphalt binder.
performance of modified asphalt. Meanwhile, it is also considered that
GO is easy to be modified by other compounds under specific conditions. 6. Discussion
In particular, its diverse oxygen-containing functional groups increase
the possibility of modification and grafting, and make it react with more Combined with the existing studies, it is possible that different 2D

Fig. 8. (a,b,c,d) are the SEM image of GO, C4H9-GO, SBS and C4H9-GO/SBS, respectively (magnified 10000X or 2000X). (e) is the schematic diagram of functional
group C4H9-GO. (f) is the synthesis mechanism of between C4H9-GO and SBS modifier. Reproduced with permission from ref. [128], Copyright 2019, Wiley Peri­
odicals, Inc. (g) is the 3D diagram of GO grafted via KH580. (h) is the reaction mechanism of among GO, KH580 and SBS modifier. Reproduced with permission from
ref. [133], Copyright 2018, Mdpi.

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J. He et al. Construction and Building Materials 330 (2022) 127222

Fig. 9. (a,b,c) are the simulation results of electron density based on between GO and saturate, aromatic and resin, respectively. Reproduced with permission from
ref. [132], Copyright 2020, Elsevier. (e ~ h) are the AFM 2D morphology of base asphalt, GOMA, SBS asphalt and SBS/GO asphalt, respectively. (i ~ l) are the AFM
2D morphology of these samples aged via PAV. Reproduced with permission from ref. [139], Copyright 2020, Elsevier.

materials, such as graphene, GNPs and GO, may have different modifi­ to bad is IAM, AAM and DAM. Because asphalt belongs to viscoelastic
cation effect on asphalt and the change of its micro morphology in material, the force between its molecules is still large in the process of
asphalt binder. There are similarities and differences among them. The high temperature preparation. However, medium solution is introduced
similarity is that graphene-like materials have similar aromatic benzene via method IAM, the asphalt binder will be in the state of solution at
ring base surface, which may show similar properties. The differences room temperature, and thus the interaction force between its molecules
are as follows: graphene structure is composed of single layer or less is also reduced, that is, in general, the molecular distance of the same
than 10 layers of ultra-thin benzene ring base surface; GNPs structure is substance in liquid is greater than that in solid [149]. Via this way of
composed of multi-layer benzene ring base surface; and GO structure is solution mixing, the contact area between them is increased, so that
based on graphene structure with rich oxygen-containing functional graphene-like materials can be more evenly dispersed in the asphalt
groups. Thus, there are still many differences in the research of nano­ binder. For the same purpose, functional groups are introduced to graft
materials modified asphalt and many contradictions in the explanation on the graphene-like materials surface to change its basic properties via
of its modification effect and mechanism. This review attempts to reveal method AAM. both IAM and AAM Methods provide new ideas for the
the modification effect and mechanism of graphene, GNPs and GO preparation of nanomaterials modified asphalt.
modified asphalt more effectively and accurately via analyzing and
summarizing the existing research of GMA, GNMA and GOMA. 6.2. Optimum content

6.1. Preparation method There is no definite conclusion on the optimal content of graphene-
like materials in asphalt binder. According to table 2-4, the minimum
The dispersion of 2D materials in composite media will directly affect dosage of it is 0.006% [131], and the maximum dosage is 6% [115]. The
the basic properties of composites [146–148]. How to improve the results show that the optimum content range of method IAM is 0.048 ~
dispersion of 2D materials in composite media is still a hot topic. Ac­ 0.53% [101,131]; that of method AAM is 0.02 ~ 1% [97,107,110,102];
cording to Table 1 and Fig. 1, there are three preparation methods for that of method DAM is 0.5 ~ 3%
GMA, GNMA and GOMA. The first is DAM, which directly adds 2D [93,103,108,117,122,130,132,136,137]. obviously, the optimum
materials into asphalt binder [93,99,103,115,117]; The second is IAM, dosage of IAM and AAM is 1 ~ 2% less than that of DAM. Therefore, the
which transforms the fusion mode of 2D materials and asphalt into so­ optimal amount of graphene-like materials in modified asphalt is greatly
lution mixing mode [101,131]; The third is AAM, which grafts and affected by its preparation method and parameters. According to the
modifies 2D materials with functional groups, and then adds them into preparation method, the order of the best dosage from large to small is
asphalt binder [96,107,110–112]. According to the dispersion effect of DAM, AAM and IAM.
2D materials in asphalt binder, the order of dispersion degree from good

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J. He et al. Construction and Building Materials 330 (2022) 127222

6.3. Effect on asphalt binder materials and asphalt binder. Some researchers think that there is
chemical reaction and physical reaction blending between the 2D ma­
There are some differences in graphene, GNPs and GO about its ef­ terial and asphalt [113,125,126,130], while other researchers think that
fects on asphalt performance, especially on the low temperature per­ there is only physical reaction but no chemical reaction between the two
formance of asphalt binder. According to the above analysis, the [97,101,128,131,132,133,135]. According to the existing research and
influence of graphene-like materials on the softening point, anti-rutting analysis, the hypothesis of that there is only physical reaction between
factor and multi-stress creep recovery rate of asphalt binder is consis­ graphene and GNPs and asphalt seems more reasonable, and the FTIR
tent, which means that the high temperature performance can be spectrum shows that the change of functional groups is only caused by
effectively improved. Moreover, it can increase the complex shear the superposition of the two functional groups, but no new functional
modulus and decrease the phase angle, that is, it can increase the storage groups appear, which means that the carbon base structure formed by
modulus and reduce the loss modulus, which means that the ability of the benzene-like structure is stable. However, the chemical and physical
asphalt to resist deformation can be effectively improved. properties of GO are more complicated due to its oxygen-containing
However, there are different views on the influence of asphalt low functional groups such as –OH, –COOH, -C– – O and –CH(O)CH–. In the
temperature. Ref. [97,101,107,111,113] and others conclude that the first case, it is considered that there is only physical reaction when it is
addition of graphene-like materials can improve the low temperature combined with SBS modifier [128,133]. In the second case, it is
stability of asphalt binder, that is, the ductility at low temperature in­ considered that there are chemical and physical reaction blending in the
creases, the stiffness modulus decreases and the m value increases, composite modification with warm mixing agent [125,126]. In the third
whereas ref. [117,118,123,137] deem that the addition of graphene-like case, it is considered that there is no chemical reaction between GO and
materials reduces the low temperature stability of asphalt binder. A asphalt, only physical adsorption without any additives [131,132]. The
possible explanation of this is that the main factor affecting the low authors think that the reason for this phenomenon is that other modi­
temperature performance is the dispersion of graphene-like materials in fiers react with oxygen-containing functional groups on GO, resulting in
asphalt binder. The former is prepared via method IAM and AAM, while the change of FTIR spectra. GO itself does not have the conditions for
the latter is prepared via method DAM, which leads to different chemical reaction with asphalt, but it still needs to be further studied.
dispersion in asphalt binder. Low temperature is different from high The current research shows that there is no clear explanation for the
temperature. When the material is stressed, low temperature often mechanism of GMA, GNMA and GOMA, but the intercalation-structure
makes the internal stress of material increase sharply [150–151]. If the hypothesis (ISH) is described by most of the literature. It is believed
2D material is not completely dispersed, it will produce agglomeration that when graphene-like materials are added to asphalt binder, their
phenomenon, and there are large agglomerates in the asphalt binder. strong adsorption on asphaltene [98] increases the interlayer distance of
When the 2D material is stressed at low temperature, it will produce asphaltene [97,101], which is conducive to the insertion of nano
obvious stress concentration, which reduces the low-temperature per­ lamellae into the lamellar structure of asphaltene, so as to play its role in
formance of asphalt. Moreover, Graphene, GNPs and GO can also be modifying the performance of asphalt [101,125]. In addition, expanded
combined with SBS modifier, rubber particles and warm mix agent to graphite is peeled off by hot asphalt to form graphene-like structure
improve the road performance of asphalt binder. For rubber particles, [102], which is considered that the strong adsorption and intercalation
the compatibility and dispersion of rubber particles in asphalt can be of asphaltene on expanded graphite sheet increases the van der Waals
increased [113,134]; For SBS modifier, the network structure of SBS force between graphite layers, resulting in the ISH. However, at present,
modifier molecules will be more stable via reacting graphene-like ma­ the ISH has not been effectively characterized and is limited to the
terials with SBS modifier molecules [107,111,114,124,133]; For warm simulation stage.
mix agent, the compaction and mixing temperature can be reduced, and In this paper, another possible hypothesis is put forward, that is,
its high temperature and low temperature performance can be substitution effect hypothesis (SEH). The SEH is that the addition of
increased. graphene-like materials play the role of asphaltene, thus changing the
performance of asphalt. When petroleum asphalt material is used as
6.4. Effect on asphalt mixture carbon precursor, graphene can be obtained via thermal decomposition
and chemical deposition method [83]. Moreover, it is believed that the
Graphene, GNPs and GO also affect the performance of asphalt disordered and irregular arrangement of PAHs forms petroleum coke,
mixture through affecting the performance of asphalt binder. When two- while the regular and orderly arrangement forms graphene [86].
dimensional materials are grafted with functional groups, the water Therefore, it is known that the two can transform each other under a
stability of asphalt mixture can be effectively improved via the intro­ certain condition, which provides a hypothetical condition for the SEH.
duction of lipophilic groups or the dense network structure with SBS According to the AFM test of asphalt, “bee structure” is often considered
modifier [114]. Moreover, the 2D material can make the smooth asphalt as asphaltene, and the edge gradual change area of its structure is
surface more rough [108], so as to improve the anti-sliding performance considered as resin [152–154]. In the colloidal model of asphalt mate­
of asphalt mixture. It is considered that the interface between the rials, it is generally considered that asphaltene is coated with resin to
modified asphalt and the aggregate is more closely combined with the form a dispersed phase, which is dispersed in the dispersion medium,
aggregate because of its rough surface modified by graphene-like ma­ that is, saturate [155–156]. In addition, the simulation in ref. [132]
terials. It is also found that there is a certain adsorption between gra­ shows that GO has the closest contact with the resin, which indicates
phene and aggregate through simulation [98]. Meanwhile, in the that the graphene-like material has the possibility of close contact with
process of preparing graphene materials with asphalt, the thin layer of the resin. At the same time, it is also considered that graphene has the
graphene coated on fine sand also has strong adsorption [78], which function of replacing asphaltene [103]. It can be clearly observed from
further increases the binding effect of aggregate and binder, so that its ref. [103 139] that the “bee structure” increases obviously after adding
water stability and anti-aging property are improved obviously. How­ graphene. The former thinks that according to the diffusion principle,
ever, at present, the research on the related mixture is still limited, and a the addition of graphene leads to the increase of this systematic viscosity
lack of research on the influence of the interface between asphalt and and the decrease of its particle fluidity, which leads to the increase of
aggregate for GMA, GNMA and GOMA still remains. number of the “bee structure”. The latter thinks that the addition of GO
promotes the binding effect of asphaltene and causes the change of “bee
6.5. Functional mechanism structure”. But the authors think that there is another possibility, that is,
the SEH. Graphene-like materials replace asphaltene and then combine
There are different views about the reaction between graphene-like with resin closely, which shows the “bee structure” in AFM images. The

19
J. He et al. Construction and Building Materials 330 (2022) 127222

“bee structure” can be observed in GMA and GOMA, which may be different modifiers, further research and demonstration are needed. It is
composed of asphaltene-resin and 2D materials-resin. The increase of known that it can increase the stability of network structure of SBS
viscosity is caused by the increase of the “bee structure” of the latter. The modifier, and also increase the compatibility and dispersion of rubber
SEH can directly explain the modification effect of graphene-like ma­ particles in asphalt binder.
terials on asphalt, which has a importance reference value. Moreover, it (4) Based on graphene and GNPs, the interaction between them and
is believed that a single hypothesis cannot be able to fully explain the asphalt is only physical reaction not chemical reaction. However, the
modification effect of graphene-like materials on asphalt, which may be reaction system of GO is controversial. It is considered that the physical
the joint effect of the ISH and SEH. reaction is the main body of the system, and whether there is chemical
reaction is affected by the addition of other composite modifiers.
6.6. Outlook and recommendation (5) Combined with the ISH, the SEH is proposed. It is considered that
the mechanism of GMA, GNMA and GOMA can be explained by both the
Most of the existing studies focused on the basic properties of asphalt ISH and SEH. The ISH is that graphene-like materials are intercalated
modified with graphene-like materials, but did not pay attention to into asphaltene to form the stacking structure of asphaltene-
other excellent properties of graphene-like materials, especially its good nanomaterial. The SEH is that the graphene-like materials act as
conductivity and thermal conductivity. In addition to the research and asphaltene and interact with resin to form the dispersed phase, namely,
development of high-performance asphalt materials, the research and the “bee structure”, which are dispersed in the dispersion medium.
development of functional 2D materials modified asphalt is another (6) In the future, more attention should be paid to the development
aspect worthy of attention. of functional modified asphalt and asphalt mixture based on graphene-
It is considered that adding graphene to asphalt can significantly like materials. Snow-melting pavement, energy-conversion pavement
improve the thermal conductivity of asphalt materials, that is, the and super-capacitor pavement are topics worth further research and
temperature can be increased to the specified range in a short time [93]. exploration.
In addition, the modified graphene is combined with petroleum asphalt
to prepare super capacitor [79], which provides a certain support for the Declaration of Competing Interest
development of intelligent pavement materials. this characteristic has
potential to be used in the research and development of snow-melt The authors declare that they have no known competing financial
pavement. In the severe cold area, when the road is blocked by ice interests or personal relationships that could have appeared to influence
and snow, the temperature of the frozen road will rise in a short time by the work reported in this paper.
heating the road, so as to achieve the effect of snow-ice melting.
Meanwhile, it can also be used for solar energy collection. Phase change References
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