Construction and Building Materials 266 (2021) 120453

Contents lists available at ScienceDirect

Construction and Building Materials

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

Review

Review on the self-healing of asphalt materials: Mechanism, affecting

factors, assessments and improvements
Bo Liang a,b,⇑, Fang Lan a, Kai Shi a, Guoping Qian a,b, Zhengchun Liu c, Jianlong Zheng b
a
School of Traffic and Transportation Engineering, Changsha University of Science and Technology, Changsha 410114, PR China
b
State Engineering Laboratory of Highway Maintenance Technology, Changsha University of Science and Technology, Changsha 410114, PR China
c
Hunan Key Laboratory for Super Microstructure and Ultrafast Process, School of Physics and Electronics, Central South University, Changsha, Hunan 410083, PR China

h i g h l i g h t s

Understanding the self-healing of asphalt materials at molecular level will benefit pavements.

The self-healing of polymer and asphalt and the factors affecting self-healing are introduced.

The evaluation and improvement methods for self-healing efficiency are summarized.

The relationship between self-healing ability and fatigue performance is discussed.

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

Article history: Fatigue cracking is one of the main diseases that affect pavement durability. Understanding the relation-
Received 23 August 2019 ship between the self-healing ability and fatigue life of asphalt materials from the molecular level will aid
Received in revised form 7 July 2020 in the preventive maintenance and improvement of asphalt pavement. This work analyzes the research
Accepted 31 July 2020
progress on the self-healing of asphalt and asphalt mixtures, including self-healing mechanism, influenc-
ing factors, evaluation methods, and improvement aspects. Factors affecting the self-healing performance
are categorized as internal, such as molecular structure, asphalt motion and diffusion, asphalt viscoelas-
Keywords:
ticity, and thixotropy, and external, such as humidity, temperature, induction conditions, and time. The
Self-healing mechanism
Molecular diffusion
self-healing performance can be adjusted by optimizing the chemical composition of the asphalt mate-
Component evaluation rials, changing the preparation method, and ensuring the spontaneous structure formation to achieve
Energy theory the intellectualization of the intrinsic material. This work sheds light on the design of materials and struc-
Self-healing enhancement technology tures for durable pavement from the perspective of the self-healing behavior of asphalt materials.
Fatigue cracking Ó 2020 Elsevier Ltd. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2. Self-healing mechanism. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1. Self-healing mechanism of polymers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.1. Thermally reversible reactions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.2. Photoreversible reactions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
2.1.3. Molecular interdiffusion. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.1.4. Reversible bond formation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2. Self-healing mechanism of asphalt . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2.1. Molecular interdiffusion. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.2.2. Capillary flow . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.2.3. Thixotropy. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
2.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7

⇑ Corresponding author at: School of Traffic and Transportation Engineering, Changsha University of Science and Technology, Changsha 410114, PR China.
E-mail addresses: liangbo26@126.com (B. Liang), lanfang1101@163.com (F. Lan), shikai94@163.com (K. Shi), Guopingqian@sina.com (G. Qian), liuzhengchunseu@126.com
(Z. Liu), zjl@csust.edu.cn (J. Zheng).

https://doi.org/10.1016/j.conbuildmat.2020.120453
0950-0618/Ó 2020 Elsevier Ltd. All rights reserved.
B. Liang et al. Construction and Building Materials 266 (2021) 120453

Nomenclature

3 PB Three Point Bending Beam Fatigue Test PAA Poly(acrylic acid)

4 PB Four-point bending test PAH Poly(allylamine)
Ar Aromatic hydrocarbons PAV Pressure aging vessel
As Asphaltene PDDA Poly(diallyldimethylammonium chloride)
AT Asphalt mixed with carbon nanotubes PEG Poly(ethylene glycol)
BBS Binder Bond Strength PEI Poly(ethylenimine)
CH2 Methylene PMA Polymer modified asphalt
CH3 Methyl PPi Pyrophosphate
CT Computed Tomography PSS Poly(sodium 4-styrenesulfonate)
DA Diels–Alder PT Phase transition temperature
DMP Dimethylphenol PVDF Poly(vinylidene fluoride)
DSC Differential scanning calorimetry R Resin
DSR Dynamic Shear Rheometry RTFO Rolling thin film oven
ESEM Environmental Scanning Electron Microscopy S Saturated hydrocarbons
FTIR Fourier Transform Infrared Spectroscopy SBS Styrene-butadiene-styrene
FTIR-ATR Fourier transform infrared spectroscopy with attenu- SDS Sodium dodecyl sulfate
ated total reflectance SMA Styrene maleic anhydride
HA Hydrogen directly connected to aromatic carbon SRR Stiffness ratio recovery
HI Healing index TEM Transmission electron microscopy
I1600 Benzene ring Tg Glass transition temperature
MD Molecular dynamics Tm Melting temperature
MIST Moisture Induced Sensitivity Test TPP Tripolyphosphate
MMF Methanol–melamine–formaldehyde TSC Two-step coacervation
MMHC Methylene plus methyl hydrogen to carbon UV Ultraviolet
MSW Medium steel wool

3. Factors affecting self-healing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7

3.1. Components and structure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.1.1. Components . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.1.2. Chemical groups . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.1.3. Activation energy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.2. Initial state before healing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.2.1. Aging level . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.2.2. Damage degree . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.3. External environment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.3.1. Time and temperature . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 8
3.3.2. Moisture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
3.4. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4. Self-healing efficiency assessment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4.1. Self-healing evaluation methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4.1.1. Performance evaluation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4.1.2. Ingredient evaluation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
4.1.3. Activation energy evaluation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4.1.4. Fatigue life evaluation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4.2. Self-healing monitor methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4.2.1. Ultrasound technique . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 12
4.2.2. Computed tomography (CT) technique . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13
4.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
5. Improvement methods of self-healing efficiency . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
5.1. Materials and methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
5.1.1. Modifier. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
5.1.2. Rejuvenator . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
5.1.3. Filler . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
5.2. Enhanced technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
5.2.1. Electromagnetic induction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
5.2.2. Microwave induction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
5.2.3. Encapsulation technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
5.2.4. Nanoparticle reinforcement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18
5.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
6. Conclusions and prospect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21

2
B. Liang et al.
1. Introduction
Fatigue crack due to repeated traffic loading is a primary distress
for asphalt pavements. [1-3]. A cracked and fatigued pavement
requires a large amount of time and energy to restore its original per-
formance, thereby requiring additional transportation and wasting
resources and causing environmental impact [4-6]. A technology that
reduces energy consumption and restores optimal pavement perfor-
mance is urgently needed in developing long-life pavements.
Self-healing has inherently hierarchical and unique multiscale
characteristics that render it as a promising approach to increase
asphalt pavement durability by healing cracks and restoring pave-
ment performance without destroying the original structure [7].
Compared with conventional maintenance techniques, self-
healing methods can remarkably reduce pavement maintenance
cost, carbon dioxide emissions, and road safety problems [8-10].
Discontinuity on the load environment causes damages or micro-
cracks inside the asphalt pavement that gradually heal only during
an intermittent period to restore its performance. Hence, the gen-
eration and healing of cracks is reversible under certain conditions.
As a viscoelastic fluid with relatively strong surface wetting and
diffusion capability, asphalt shows a self-healing behavior that can
close its microcracks and therefore restore its stiffness and
strength. Asphalt self-healing can improve the fatigue cracking
performance of asphalt pavements. Cracks can be closed when
the entire self-healing process is completed; therefore, asphalt
materials must have a good self-healing ability [11,12]. Composite
designed has changed greatly due to the discovery of intrinsic self-
healing polymers, that is, polymers that can recover mechanical
bonding with themselves or other materials. Traditional matrix
and intrinsic self-healing polymers show potential as binders that
combine the healing ability and acceptable mechanical properties.
The self-healing performance of asphalt materials is beneficial
to their lifetime, which is strongly influenced by their molecular
structure and certain environmental conditions. Herein, internal
inherent factors such as molecular composition, structure, asphalt
movement and diffusion, asphalt viscoelasticity, and thixotropy
and external factors such as humidity, temperature, induction con-
ditions, and self-healing duration are comprehensively considered
and qualitatively and quantitatively evaluated from the perspec-
tives of molecular structure, molecular motion mechanism, asphalt
physical properties, research methods, and test conditions. The
influence of material modification and processing technology on
the self-healing performance of asphalt and asphalt mixtures is
also analyzed in detail. This work aims to provide a systematic
design of self-healing asphalt materials with high-performance
for durable pavement construction.
2. Self-healing mechanism
Self-healing materials can heal themselves either sponta-
neously or after activation and ultimately restore diverse proper-
Fig. 1. Schematic representation of intrinsic self-sealing by using external stimuli [19].
3
Construction and Building Materials 266 (2021) 120453
ties, such as mechanical, optical or electrical properties. Self-
healing principles have been expanded from chemistry to engi-
neering [13-16].
2.1. Self-healing mechanism of polymers
Self-healing polymer materials show promising applications.
Reversible polymers have common reversibility during polymer-
ization and cross-linking [17,18]. Intrinsic self-healing is driven
by macromolecular interactions. Asphalt is considered a complex
polymer, and its self-healing mechanism must be derived from
that of polymers. An external trigger, such as thermal, photochem-
ical, and electrical effects, is important to enhance this process
(Fig. 1). Effectively and autonomously restoring their function is
the challenge for self-healing functional materials.
2.1.1. Thermally reversible reactions
According to the concept of time/thermally reversible viscosity,
a precipitous drop in viscosity occurs upon heating and damage
repair by external stimuli. Upon cooling, the local properties (e.g.,
viscosity) are restored to initial values [19]. Chen et al. [20]
designed healable polymers with thermal reversibility through
the concept of self-healing. These highly cross-linked polymeric
materials were synthesized with multifuran and maleimide via
the Diels–Alder (DA) reaction. Intermonomer linkages disconnect
(corresponding to the retro-DA reaction) above 120 °C and then
reconnect upon cooling (i.e., DA reaction) as shown in Fig. 2 (a).
This fully reversible process exhibits a 57% recovery rate of fracture
toughness. These polymers possess mechanical properties compa-
rable with those of commercial epoxy and unsaturated polyesters
[21,22].
Canadell et al. [24] incorporated disulfide link to a rubber net-
work to fully restore its failure strain at moderate temperatures
(e.g., 60 °C). Self-healing occurs above the material’s T g because
of the chain segments’ mobility to enable interchange reaction.
This method can be used for materials with low T g , such as polyur-
ethanes and polyesters.
2.1.2. Photoreversible reactions
Photoreversible reactions can also realize polymer self-healing
[18]. Photochemical [2 + 2] and [2 + 4] cycloadditions are the most
common photodimerization reactions used for polymer photo-
chemical healing because of the cycloaddition reversion that
results in C = C bonds and readily occurs in the solid state [25].
Cyclobutane reverses to the original cinnamoyl structure upon
crack formation and propagation. Crack healing can also be accom-
plished through the recycloaddition of cinnamoyl groups as shown
Fig. 2(b).
Other reversible chemical reactions, such as disulfide bonds, liv-
ing silicone, transesterification exchange, dynamic C–C bond
exchange, and reversible C–ON bonds, have been developed. These
mechanisms with reversible covalent bonds have expanded the
B. Liang et al.
Fig. 2. (a) Thermoreversible and healable fiber-network interface (maleimide
functionalization of the glass fiber within a furan-functionalized polymer network)
[21] and (b) mechanism of fracture and repair of photo-induced healing [23].
family of intrinsic self-healing materials and provided additional
choices for various requirements.
2.1.3. Molecular interdiffusion
Polymer crack healing via molecular interdiffusion has been
studied since the 1980 s [26,27]. According to Wool and O’ Con-
nor’s pioneering work on polymer healing, healing consists of the
following five stages: (1) surface rearrangement, (2) surface
approach, (3) wetting, (4) diffusion, and (5) randomization. The
healing mechanism related to intermolecular diffusion is illus-
trated in Fig. 3(a).
The healing function consists of two parts, namely, the strength
gain caused by instantaneous cohesion between wetting crack
sides and by intermolecular diffusion between crack sides. The
cracks heal immediately after the external loads are removed.
Two phenomena exist, namely, the viscoelastic recovery of bulk
materials and the healing of the crack zone. The difference
between these two is that the former is caused by molecular rear-
rangement, and the latter is the result of wetting and mutual diffu-
sion on both sides of the crack [31].
Fig. 3. (a) Mechanisms involved in self-healing via molecular interdiffusion [28]; (b) Healing of a crosslinked network via dangling chain entanglement [29]; (c) Theoretical
healing mechanism in ionomers [30].
4
Construction and Building Materials 266 (2021) 120453
Wool et al. [26,27] confirmed that crack healing in thermoplas-
tics occurs most effectively at or above the materials’ T g . The inter-
face gradually disappears when two identical polymers come into
contact at a temperature higher than T g . The mechanical strength
of the polymer–polymer interface then increases, and the cracks
heal gradually due to molecular diffusion at the interface. As deter-
mined by the recovery of tensile strength, the healing degree
depends on wetting and diffusion. [32]. Little and Bhasin [33] pro-
posed that when the two sides of the crack come into contact, the
molecule diffuses from one side to the other until the crack disap-
pears. In addition, the healed material reaches the strength level of
the raw material. Therefore, this ability depends on the material’s
surface energy and the diffusion and random ability of the
molecules.
2.1.4. Reversible bond formation
End-group recombination of polymers is a relatively new tech-
nology for repairing structural (strength loss) and molecular (chain
breakage) damages of some thermoplastics. The chain mobility in
thermoplastics can be used to heal fractures at ambient tempera-
tures by introducing reversible bonds in the polymer matrix. This
method uses H or ion bonds to repair damaged polymer networks
and is an alternative to covalent bond healing initiated by ultravi-
olet rays or catalysts [34]. The chain rearrangement repair cracks at
room temperature are shown in Fig. 3(b). Harreld et al. patented a
system exhibiting molecular self-healing via reversible bond for-
mation [35]. The healing time can be adjusted by changing the
polymer structure, the crosslinking degree, or the crosslink
strength. The crosslinked component includes a polymer domain
containing intermediate strength crosslinks formed by hydrogen
and/or ion bonds, which enhance the self-healing efficiency as
shown in Fig. 3(c).
Polymer with strong intermolecular forces fills the cracks and
pulls each other, thereby restoring the original performance. A
composite material consisting of 70 wt% metal salts of sulfonated
poly(ether ketone) (M = sodium or zinc) and 30 wt% sodium oleate
(NaOl) was prepared [36], and the ionic nanodomains formed by
the interaction of ionic groups provide a physically cross-linked
network and strong dipolar interactions between the ionomer
and the dispersed crystalline NaOl. Shape was recovered by reheat-
ing the material over its T m without applying stress and achieved
shape fixing efficiency of 96% and shape recovery of 100%.
2.2. Self-healing mechanism of asphalt
2.2.1. Molecular interdiffusion
Asphalt self-healing mechanism is a comprehensive behavior
with many factors because of its complex chemical composition.
Asphalt binders can repair themselves or recover minor damage
B. Liang et al. Construction and Building Materials 266 (2021) 120453

during the load cycle. The chemical properties of asphalt, such as
chain length and branches, can affect its self-healing. One of the
healing mechanisms is molecular self-diffusion across the crack
interface [37].
Molecular dynamics (MD) computer simulation considers the
atom and/or molecule interaction on the basis of physics laws
[38]. MD was derived from the theory proposed by Wool et al.
[28,39] and is widely applied in asphalt materials [40,41]. An inter-
face system was created by adding a vacuum pad of 10 Å on one
side of a unit amorphous cell and a layer with artificial crack rep-
resenting the self-healing interface to determine the self-healing
property of the asphalt binder. Fig. 4(a) and (b) show the MD
model to simulate the diffusion of molecules across a crack inter-
face. According to the simulation results, the asphalt molecules
have diffused across the artificial crack interface, and crack healing
could be observed. The calculated diffusion coefficient was used to
evaluate the healing capability of the asphalt binders [42].
Molecular diffusion plays an important role during self-healing.
An increase in diffusion coefficient accelerates the self-healing per-
formance of asphalt; therefore, this parameter is introduced to
evaluate the self-healing capability of asphalt binders. The molec-
ular diffusion rate strongly influences the self-healing ability of
asphalt. According to MD simulation, the diffusion coefficient of
neat asphalt is higher than that of SBS-modified asphalt when
the temperature is below 273 K. At this temperature (near the glass
transition temperature), the asphalt binder behaves similarly to a
non-Newtonian fluid. The diffusion coefficients of the SBS-
modified asphalt are higher than those of the neat asphalt at sim-
ulation temperatures higher than 273 K. This result indicates that
SBS modification strongly affects the healing potential of asphalt
based on the diffusion coefficient [44].
High temperature facilitates the self-diffusion of asphalt mole-
cules and provides kinetic energy for fast molecular movement
[41]. The density and T g of the base asphalt and SBS-modified
asphalt binders were initially analyzed via the MD simulation.
The diffusion coefficient of the SBS-modified asphalt is higher than
that of the base asphalt and increases with the temperature as
shown in Fig. 4(c–e). At different temperatures, the healing index

Fig. 4. Effect of molecular diffusion on asphalt self-healing. (a) Layered structure of two amorphous cells with interfaces; (b) Layered structure after being subjected to
accelerated healing at elevated temperatures [37,42,43]; (c) Diffusion coefficients of asphalt binders at different temperatures (106 cm2/s); (d) Diffusion coefficient versus
simulation temperature plot, and (e) ln (HI) versus T1 for neat and styrene–butadienestyrene (SBS)-modified asphalt binders [42].

5
B. Liang et al.
(HI) value of the SBS-modified asphalt is higher than that of the
base asphalt. The MD model and force field of asphalt provided
accurate methods for predicting the asphalt binder performance.
2.2.2. Capillary flow
Intermolecular diffusion cannot occur when a large gap exists
between the new cracks in asphalt. However, if a period of rest is
allowed and sufficient energy is applied to the asphalt material,
then healing can continue, and the visible cracks will disappear.
Considering that the healing theory based on molecular diffusion
and reversible bond formation is not applicable, the healing theory
based on the capillary flow is proposed to explain crack healing in
asphalt pavement. Contact points and gaps are observed when the
crack surface is in contact. If the binder behaves similarly to a New-
tonian fluid, then a pressure difference is observed at the contact
point and may act as the driving force for the capillary flow of
the asphalt binder. Under suitable temperature conditions, the
capillary flow in asphalt cracks will lead to crack closure [45,46].
The capillary phenomenon can be studied by modifying the
simplified Lucas–Washburn equation (Fig. 5) [47]. If the asphalt
concrete temperature is high enough to make asphalt behave as
the Newtonian fluid, capillary phenomena will begin at the point
of contact between the two cracks. Asphalt will flow through any
possible crack in the form of capillary flow and will heal when
the temperature is higher than the temperature threshold [64].
Therefore, at a certain period of time, increasing the temperature
Fig. 5. Scheme of the forces acting in an asphalt mixture crack during healing [47].
6
Construction and Building Materials 266 (2021) 120453
above the Newton transformation temperature is the most appro-
priate way to repair asphalt mixture [48].
2.2.3. Thixotropy
Thixotropy is the tendency of those fluids that exhibit reversible
structural changes due to the molecular rearrangement in the bitu-
minous phase [49,50]. Thixotropy and self-healing occur simulta-
neously when a bituminous material is subjected to an external
stress [51,52]. The asphalt thixotropy originates from the evolution
of interactions (weak bonds) at the molecular or macromolecular
scales. Thixotropy has been applied to describe the non-
Newtonian behavior of asphalt cement at high temperatures
[53,54]. Asphalt thixotropy means that with the increase of loading
time, the asphalt viscosity decreases gradually, and when the load
stops, the asphalt viscosity recovers. The decrease and increase of
viscosity are due to the microstructure destruction and reorganiza-
tion. This phenomenon is similar to the fatigue and self-healing of
asphalt, i.e., the failure and reorganization of microstructures.
Macroscopically, this situation shows the decrease and increase
of parameters, such as modulus and viscosity. Thixotropy results
in structural changes during oscillation cycles (e.g., in frequency
domain) and in long transients, which can affect the fatigue and
healing of the asphalt binder subjected to oscillatory loading
[55]. Soltani and Anderson [56] used a uniaxial ‘‘push–pull” test
with three loading stages on a cylindrical specimen to study the
fatigue and healing. The effects of self-heating, self-cooling, and
B. Liang et al.
nonlinear non-fatigue phenomena are discussed. The main part of
the modulus loss in fatigue test and the modulus obtained during
rest or load reduction are the thixotropy results.
2.3. Summary
Asphalt is a viscoelastic polymer with self-healing ability. Con-
sidering environmental and material properties may help in pro-
moting the self-healing of asphalt mixtures.
3. Factors affecting self-healing
The asphalt self-healing efficiency depends on the physico-
chemical properties, damage degree, and external conditions such
as temperature and time. The schematic diagram of influencing
factors on asphalt self-healing efficiency is shown in Fig. 6.
3.1. Components and structure
3.1.1. Components
The characteristics of asphalt and its ability to interact with
other materials are affected by its four components [57]. Four-
component method is used to analyze the asphalt healing index
(HI). Four components of asphalt are divided into asphaltene
(AS), saturated hydrocarbons (S), aromatic hydrocarbon (Ar), and
resin (R). Grey relational analysis of the four components and
self-repairing performance of the asphalt is carried out, and the
descending order is as follows: Ar > S > R > As [58]. The self-
healing ability can be improved by increasing the ratio of saturates
with long aliphatic chains to aromatic hydrocarbons with the main
dense ring structures. As shown in Fig. 7(a), the S/Ar value
increases from 0.26 to 0.28, and the HI value increases from 0.25
to 0.35. The percentages of asphaltenes and resins can well repre-
sent the content of large molecule. With the presence of several
large molecules, the average molecular weight is also large. As a
result, the asphalt molecular motion is slow, and the self-healing
ability is poor. Therefore, the asphalt crack takes a long time to
heal.
Fig. 6. Schematic diagram of influencing factors on self-healing efficiency.
7
Construction and Building Materials 266 (2021) 120453
3.1.2. Chemical groups
The benzene ring (I1600) content and the ratio of methylene
(CH2) and methyl (CH3) are important indices to evaluate the
chemical structure of asphalt binders [37]. Long chains with few
branches can move at the crack interface and promote healing.
High CH2/CH3 value indicates low content of the branched chain
in the asphalt molecule and low high H content asphalt molecular
branch chain directly connected with aromatic carbon (HA). Thus, a
long and thin molecular structure is formed. These molecules exhi-
bit a smaller hindering effect and diffuse faster than other mole-
cules. In addition, bitumen binders tend to rapidly heal the
microcracks. HI increases with CH2/CH3 and HA as shown in
Fig. 7(b) and (c) [58].
Methylene plus methyl hydrogen to carbon (MMHC) ratio iden-
tifies the branching degree of the aliphatic or chain structures. The
self-healing efficiency decreases when the MMHC value increases
[37,59]. The I1600 content negatively affects HI. High I1600 content
in asphalt indicates a high molecular weight, thereby leading to
the low-efficiency molecular diffusion rate as shown in Fig. 7(d)
(e). As a result, self-healing requires a long time.
3.1.3. Activation energy
Energy substantially affects self-healing efficiency. When suffi-
cient energy is transferred to the system, molecules carrying
enough kinetic energy can cross the activation energy barrier,
wet the fracture surface, diffuse from one surface to another, and
finally close the crack. Activation energy is defined as the mini-
mum energy required in the chemical reaction. The key factor is
to overcome the activation energy barrier of self-repair [60]. Low
activation energy means fast self-healing rate. When microcracks
are formed, the asphalt molecules can wet both sides of the cracks
and make the two sides of the cracks fully contact under the
increasing temperature. However, microcracks can merge into
macrocracks with damage development. The activation energy
barrier becomes exceedingly high for asphalt molecules, thereby
leading to self-healing failure [61].
The healing activation energy must be determined first to eval-
uate the self-healing ability of the asphalt mastic [60]. The self-
healing ability is largely dependent on the damage degree of the
B. Liang et al.
Fig. 7. Impact factors of self-healing. (a) Correlation between S/Ar and HI [58]; (b) Comparison of CH2/CH3 ratio of binders created using average molecules to self-diffusivity
of molecules at crack interface[37]; (c) Relationship between HA and HI [58]; (d) Relationship between healing and molecular characteristics of asphalt binders [37]; and (e)
Relationship between I1600 and HI [58].
asphalt mastic. Thus, fatigue–rest–fatigue test under different rest-
ing times and temperatures must be conducted at a certain dam-
age degree. The activation energy of self-repair is related to the
types of asphalt materials and original damage types. If the surface
energy of asphalt is equal to or greater than the self-healing
energy, then self-healing occurs. The activation energy of the
asphalt flow is greatly influenced by different sources and aging
levels of the asphalt materials. On the basis of the complete recov-
ery time and healing activation energy of asphalt at a given tem-
perature, the equivalent healing time can be calculated at
different temperatures [45,62].
3.2. Initial state before healing
3.2.1. Aging level
Bhasin et al. [63] studied the percentage of healing of the three
asphalt binders at different temperatures and aging conditions. The
stiffness of the test specimen after rolling thin film oven (RTFO)
aging is restored to 75% of the original, whereas the stiffness of
the test specimen after pressure aging vessel (PAV) aging is
restored to 60% after standing for 60 min at 20 °C. A 60% gain in
stiffness is the maximum self-healing capacity of the asphalt bin-
der considering that the microcracks are completely and instanta-
neously reversed upon formation. Aging of the asphalt binder
decreases the intrinsic healing rate (Fig. 8(a)).
To further understand the effect of aging on self-healing effi-
ciency, Xu et al. [43] investigated the oxidative aging effect of
the asphalt binder by using MD simulation. Aging weakens the
nano-aggregation behavior of the AS molecules and reduces the
translational mobility of the asphalt molecules. The molecular dif-
fusion of the aged asphalt decreases due to the increase in molec-
ular size in AS, R, and aromatic and reduced free volume for
saturation.
8
Construction and Building Materials 266 (2021) 120453
3.2.2. Damage degree
The damage degree represents the reduction of the effective
load-carrying area due to repeated use of the load. Therefore, the
damage degree is directly related to the width and density of the
crack, and a high damage degree requires great self-healing energy.
At high temperature and low damage level, the fracture damage is
quick and easy to heal [60,64].
Four groups of specimens are used to analyze the horizontal
effect of damage. The fatigue damage level of the first group is
defined as the decrease of bending stiffness modulus to 50% of
the initial value. When the specimen is loaded 50 times, the initial
stiffness modulus is defined as the stiffness modulus. The three
other groups have the same test procedure, but the damage degree
is 60%, 70%, and 80% of the initial value, correspondingly [61]. Fig. 8
(b) displays the influence of the damage level of the asphalt mix-
ture beams on the recovery rate of the stiffness modulus and fati-
gue life extension ratio. The fatigue life prolongation rate decreases
from 1.33 to 0.24 when the damage degree decreases from 50% of
the initial stiffness modulus to 60%. With the increase of damage
degree, the recovery rate of the stiffness modulus also decreases.
However, the decrease range is less than the fatigue life prolonga-
tion rate. When the number and size of microcracks are within a
certain range, the microdamage can be effectively recovered.
Under continuous fatigue loading, the microcracks will continue
to increase. When the fatigue load continues, considering the dam-
age accumulation, the microcrack will become a macrocrack, and
the asphalt mixture damage will be difficult to repair.
3.3. External environment
3.3.1. Time and temperature
Asphalt is a viscoelastic polymeric material with time–tempera
ture-dependent behavior [65]. Healing levels increase with the
B. Liang et al. Construction and Building Materials 266 (2021) 120453

Fig. 8. (a) Total intrinsic healing at 60 min as a function of temperature and aging [63]; (b) Effect of damage level on healing efficiency [61]; (c) Strength recovery ratio at
different heating temperatures [66]; (d) Induction heating versus healing recovery [67]; and (e) HI as a function of temperature [68].

extension of standing time, healing speed, and temperature level.
The time–temperature characteristics of self-healing were also
investigated [66]. Fig. 8(c) shows that heating the crack beam at
below 20 °C does not lead to any healing. With the heating temper-
ature increasing from 30 °C to 85 °C, the recovery fracture resis-
tance of the beam increased from 14.9% to 78.8%. However,
heating the sample further to 100 °C will lead to a decreased heal-
ing rate. Similar results were obtained by Mengzi et al. [67]. HI of
the asphalt samples undergoing 2826 cycles of testing and differ-
ent periods of induction heating are shown in Fig. 8(d). The natural
healing of samples reaches 11% without induction heating. Addi-
tionally, after 8 s heating time at 55 °C, approximately 30% of the
healing recovery is reached.
Fig. 8(e) also shows the healing index reaching its peak when
the temperature is increased to a certain extent. A long heating
time may lead to expansion and binder drainage problems, thus
reducing the healing efficiency [69]. The influence factors of tem-
perature on the self-healing properties of different bitumen bin-

9
B. Liang et al.
Fig. 9. Effects of healing time and water on the healing capability of bitumen [74].
ders are similar. Under optimum induction temperature, the max-
imum self-healing rate does not affect other performances. The
phase transition temperature (PT) range of the asphalt binder can
be measured by differential scanning calorimetry. In the PT range,
the MD rate and diffusion range of asphalt are obvious, and the
asphalt self-healing ability is strong.
The influence factors of temperature on the self-healing proper-
ties of different bitumen binders are similar. Under the optimum
induction temperature, the maximum self-healing rate does not
affect other performances. The PT range of the asphalt binder can
be measured by DSC. In the PT range, the MD rate and diffusion
range of the asphalt are obvious, and the asphalt self-healing abil-
ity is strong.
3.3.2. Moisture
When water molecules enter the asphalt concrete, they will dif-
fuse at the molecular level into asphalt binders, leading to the
cohesive failure of asphalt and adhesive failure between the
asphalt and aggregate [70,71]. Therefore, asphalt binder healing
is highly sensitive to moisture regulation.
Sun et al. [72] studied the healing properties of asphalt concrete
with moisture damage. The thermal conductivity of asphalt mix-
ture increases with the increase in water content, whereas the
thermal diffusivity and specific heat decrease. Thermal healing
can only partially recover the healing strength, whereas the struc-
tural deformation caused by water damage cannot be repaired by
heating technology. Mannan et al. [73] used moisture-induced sen-
sitivity test to evaluate the moisture condition effects on the bin-
ders. High temperature (60 °C) and pressurized (40 psi) water
were forced into the asphalt binder, thereby accelerating the bin-
der moisture conditioning. The Fourier-transform infrared spec-
troscopy (FTIR) results showed that the content of the hydroxyl
group in asphalt was increased by water regulation. When mois-
ture is absorbed in the binder, high energy is required for the dif-
fusion on microcrack surfaces, thereby diminishing the long-term
healing of the binder.
Lv et al. [74] also reported that water has multiple effects on the
healing potential of bitumen. The amount of healing measured
under dry conditions increases as a logarithmic function of healing
time, whereas the healing ratio of bitumen under wet conditions
increases over time and then decreases (Fig. 9). The good affinity
of the H atoms in water with the Lewis acid and base components
of the surface energy results in strong H bonds and enhanced the
10
Construction and Building Materials 266 (2021) 120453
healing capability. The bonding of the H atoms takes a long time.
Therefore, this interaction can improve the long-term healing
potential of bitumen. Water also shows a negative influence when
the strength steps over a peak value.
3.4. Summary
The movement of asphalt molecules is related to its molecular
structure and some external factors. For example, self-healing
time, temperature, humidity, and destruction degree have multiple
effects on the self-healing efficiency. All kinds of factors must be
comprehensively considered in choosing the best self-repair condi-
tion. Table 1 summarizes the effect factors on asphalt self-healing
efficiency.
4. Self-healing efficiency assessment
The evaluation indexes include different fatigue tests with dif-
ferent rest times because pavement healing is usually related to
microcracks and fatigue damage. The basic self-healing evaluation
methods are to measure the change or recovery of material prop-
erties before and after self-healing. Different experimental meth-
ods, such as DSR, MD [42] and FTIR [59], indirect tensile fatigue
test (ITFT) [67,78], binder bond strength (BBS), and three point
bending beam fatigue test (3 PB) [79], are used to determine the
change in properties of the asphalt materials before and after heal-
ing. These methods are based on different evaluation factors, such
as complex modulus, activation energy, MMHC, fatigue life, and
strength. By means of ultrasonic or computed tomography (CT)
technique, the change of internal gaps in the asphalt mixture can
be detected to estimate the growth or closure of cracks. The indica-
tors for evaluating the self-healing efficiency at different scales are
shown in Fig. 10.
4.1. Self-healing evaluation methods
4.1.1. Performance evaluation
Modulus and strength are two main properties of asphalt mate-
rials [81,82]. The performance characterization of asphalt before
and after rest period is the most commonly self-healing evaluation
method. Lv et al. [59] used bond strength test to evaluate the self-
healing ability of the modified asphalt binder. BBS test indicates
B. Liang et al. Construction and Building Materials 266 (2021) 120453

Table 1
Summary of influencing factors and their effects on healing efficiency.

Factors Note References

Components and structure S/Ar The value increase indicates the molecular structure tends to be slender. [58,75]
CH2/CH3 The ratio increase means molecular diffusion rate accelerated. [37,76]
HA High HA content has less branched chain, thereby resulting in long and thin molecular [58]
structure
MMHC The ratio increase indicates the deceleration of molecular diffusion rate. [37,59]
I1600 The I1600 has a large molecular weight. Increased molecular weight decreases diffusion [37,58]
rate
Activation energy Self-healing efficiency decreases with increasing activation energy [42,45,73]
Initial state before healing Aging level The molecular diffusion of aged asphalt decreases [43,50,63,74]
Damage degree Healing rates will decrease with the crack width [64,68,77]
External environment Temperature The self-healing efficiency reaches the maximum when the temperature is heated to a [45,63,67,74]
certain temperature. Temperature is exceedingly high, the healing level of asphalt test
samples decreases.
Healing time The self-healing level increases as the rest time increases. [45,73,74]
Moisture Water exerts multiple effects on the healing potential of bitumen. It negatively influences [73,74]
the healing capability over time.

   
that the modifier significantly affected the healing potential of the where Ginitial  is the initial modulus value; Gterminal  is the modulus
 
asphalt binder. The increase of modifier content reduces the heal-  
ing ability of basic adhesive, which is independent of the type of
additive. This result indicated that soft adhesive is suitable for
healing. Four-point bending test (4 PB) test further confirmed that
bond strength test can help determine the healing potential of the
asphalt binders in an efficient and simple manner. The experimen-
tal process includes three steps: preparation of the asphalt speci-
mens, fatigue self-healing (F-H) cycle, and tensile test. The self-
healing index is based on Eq. (1), as follows:
POTSAi
HIi ¼ ð1Þ
POTSi
where HIi is the healing index after the i cycles of F-H; POTSAi is the
recovered pull-off tensile strength after the i cycles of F-H, and
POTSi is the initial pull-off tensile strength before healing.
In 2016, Sun et al. [42] adopted fatigue self-healing fatigue test
to evaluate the asphalt self-healing performance based on the
change of modulus. The threshold of damage degree is set at
30%, that is, the loading stops when the initial modulus drops to
70% of the initial value. The formula for Eq. (2) is shown as follows:
 
jG jhealing  jG jterminal
HIG ¼ ; ð2Þ
jG jinitial  jG jterminal
Fig. 10. Evaluation index of self-healing efficiency under different scopes [42,59,67,79,80].
11
value when the loading stops, and Ghealing  is the initial modulus
value after rest.
The effectiveness of the evaluation index depends on the heal-
ing temperature and rest time, and the healing ability of different
asphalt materials can be classified under certain conditions. Pre-
dicting the time-dependent healing at different healing tempera-
tures is difficult. Therefore, establishing a universal self-healing
evaluation index on the basis of self-healing is necessary.
4.1.2. Ingredient evaluation
Some defects are observed in the method of evaluating self-
healing ability of asphalt only from the performance. The develop-
ment of self-healing evaluation index based on the intrinsic prop-
erties of materials is another method to evaluate the asphalt self-
healing ability. The MMHC ratio is a useful index in predicting
the healing potential of the base asphalt binder by using Eq. (3)
[76]. The MMHC viability was used to characterize the healing
capabilities of different asphalt binders via FTIR.
A1380
þ A2920
HCH3 þ HCH2
MMHC ¼ ¼ A5 7
ð3Þ
CCH3 þ CCH2 1380
þ A2920
15 14
B. Liang et al. Construction and Building Materials 266 (2021) 120453

where A1380 is the –CH3 symmetrical stretch absorption from

1385 cm1 to 1365 cm1; A2920 is the –CH2 asymmetrical stretch
absorption from 2936 cm1 to 2916 cm1; The 5, 7, 14, and 15
are the constants for the numbers of H and C based on the func-
tional group atomic weights; HCH3 is the H atom content in methyl;
HCH2 is the H atom content in CH2; C CH3 is the C content in CH3;
and C CH2 is the C atom content on CH2.
HI decreases with the increase in MMHC ratio of the asphalt
binder, indicating good healing performance of base binders with
long aliphatic chains. However, the MMHC ratio is unsuitable for
modified asphalt.

4.1.3. Activation energy evaluation

The viscous flow process can be considered a thermal process,
where atoms, groups of molecules, and molecules should move
by overcoming an energy barrier [32]. According to the Arrhenius
law, the activation energy of asphalt molecule movement can be
used as a self-healing index to evaluate the self-healing ability of
base and modified asphalt [45,60]. The HI value is logically equiv-
alent to the diffusion coefficient. HI is a macroscale indicator used
to evaluate the healing behavior of the asphalt binders from a
macroscopic view. The diffusion coefficient is a microscale indica-
tor, which can be obtained from the MD simulation. The activation
energy is calculated with the temperature and the universal gas
constant, as shown in Eqs. (4) and (5) as follows:
Eh
HI ¼ Aexpð Þ ð4Þ
RT
Eh
D ¼ Aexpð Þ ð5Þ
RT
where A is the pre-exponential factor; Eh is the activation energy,
and R is the universal gas constant (8.314 J/mol/K).
The healing activity of different asphalt adhesives is obviously
different. Healing activation energy represents the minimum
energy required to increase the time-dependent intensity. Activa-
tion energy can reflect the effect of asphalt type, filler type, and fil-
ler content on the curing of asphalt adhesive. Eh can classify the
healing ability of different bitumens in a time-dependent manner.
The effective healing time at different temperatures can be calcu-
lated by the complete healing time of asphalt at reference temper-
ature and the activation energy.
4.1.4. Fatigue life evaluation
Healing process can be hypothesized to be the reverse process
of cracking, which involves two important phases, namely, crack
closure and strength gain [83,84]. As shown in Fig. 11 (a) and
(b), cracking occurs due to the cohesive fracture of asphalt binder
or emulsion phase and the adhesion fracture of asphalt binder and
aggregate interface [85,86]. Enhanced self-healing capabilities can
accelerate the closure of fractures and restore material strength.
3 PB and 4 PB tests are commonly used to evaluate the perfor-
mance of asphalt mixtures before and after self-healing. Dai et al.
[88] used fracture-self-healing tests to determine the self-healing
capacity of asphalt mastic and asphalt mixes in an improved
3 PB via the elastic support and self-healing procedure. Shirzad
et al. [89] measured the flexural stiffness of the prepared beam
samples by using the 3 PB setup. By comparing the initial stiffness
and the stiffness at days 0 and 6, the self-healing progress of the
beam was evaluated on the basis of the stiffness ratio recovery
rate. Results showed that the mixtures containing sunflower oil
had the best self-healing effect.
The damage content in the subsequent healing test is calculated
using the fatigue life of the beams under different strain levels via
the 4 PB test [69]. The test process includes damage 4 PB fatigue
Fig. 11. Relationship between self-healing and fatigue life. (a) Failure mode of
cracking in asphalt mixture [87] and (b) diagram of the three-step healing
mechanism in bitumen [51].
test in which flexural stiffness is reduced by 50%. The fatigue life
of the second cycle indicates healing caused by rest and induction
heating. As shown in Fig. 12 (a), the relative healing indication
eliminates the influence of the absolute fatigue life on the healing
rate.
Fig. 12 (b) illustrates the fatigue life extension changes as a
function of resting and heating temperature through the 4 PB test.
The increase in fatigue life extension ratio indicates that healing is
induced. Healing is greatly improved when the heating tempera-
ture increases from 70 ℃ to 85 ℃. The fatigue life extension ratio
decreases due to the increase in temperature, and the geometric
damage is caused by overheating. The fatigue life extension ratio
reaches its peak at 85 ℃, which is verified as the optimum heating
temperature.
Repeated repair ability, which is related to the durability of
pavement, must be considered to ensure the sustainable use of
self-healing materials. Microcapsule/asphalt composites have mul-
tiple self-healing capabilities [10]. Garcia et al [48] induced fivefold
damage and healing on asphalt mixture specimens and proved that
healing can be repeated, but the mechanical properties of the
asphalt concrete decreased after each healing. The effects of sun-
flower oil microcapsules with different particle sizes and core
materials on the repeated repairing ability of the filling material
were evaluated, and the results confirmed that the modified
asphalt material has a good multiple repair capability [91].
The detailed evaluations of self-healing efficiency according to
different indicators are summarized in Table 2.
4.2. Self-healing monitor methods
4.2.1. Ultrasound technique
As a non-destructive control method, acoustic emission is used
to evaluate material damage in many fields. Advanced techniques
by using neural networks for ultrasonic detection can rapidly and
effectively evaluate the damage state of the asphalt mixture under
different temperatures and water contents during water–tempera
ture–radiation cycles [80]. The model established by the support
vector machine has high accuracy and stability and can reflect

12
B. Liang et al. Construction and Building Materials 266 (2021) 120453

Fig. 12. Effect of healing on fatigue life. (a) Definition of fatigue life extension ratio [69] and (b) fatigue life extension ratios of samples with different resting and heating
temperatures [90].

Table 2
Evaluation of self-healing efficiency according to different indicators.

Factors Formula Meaning/Note Test method References

Fatigue life N p N0:5 NP: cycles; N0.5: cycles with a 50% probability of ITFT [67,92]
HI ¼ N0:5
breaking the test samples before healing
Tensile strength HIi ¼ POTSAi HIi: self-healing index after i F-H cycles; POTSAi: recovery of 3 PB; BBS [74,79]
POTSi
tensile strength after i F-H cycle; POTSI = initial tensile
strength before self-healing.
Complex modulus HIG ¼
jG jhealing jG jterminal
HIG ¼
jG jhealing jG jterminal jG jinitial : initial complex modulus; jG jinitial jG jinitial : modulus DSR [42]
jG jinitial jG jterminal jG jinitial jG jterminal
of 2 min shearing. jG jhealing : the complex modulus after
healing, jG jterminal = 70%jG jinitial
Force h ¼ FðtÞ F0: ultimate force by 3 PB, F(t): ultimate force 3 PB [45]
F0
measured in the beams after healing
Dissipated energy DEn DEm RDECn: ratio of dissipated energy change value at Nth cycle; [93]
RDECn ¼ DEm ðnmÞ
DEm, DEn: dissipated energies at the mth and nth cycles; m < n
Stiffness SRR ¼ Measuredstiffnessatday0or6 SRR: stiffness ratio recovery 3 PB [89]
Initialstiffness
Crack width i widthc light microscopyand [89]
Hi ¼ Width
Width
 100% Widthi: Initial crack width; Widthc : Crack width curing
i
image analysis
MMHC HCH3 þHCH2
A1380 A2920
þ A1380: –CH3 symmetrical stretch from 1385 to 1365 cm1, FTIR [59]
MMHC ¼ ¼ A1380
5 7
C CH3 þC CH2
A2920: –CH2 asymmetrical stretch from 2936 to 2916 cm1, 5,
A2920
15
þ 14

7, 14, 15: the numbers of H and C based upon functional

group atomic weights.
Activation energy Eh A: the pre-exponential factor, Eh: is the activation energy, R: MD [42]
HI ¼ Aexpð RT Þ
the universal gas constant (8.314 J/mol/K).

the relationship between ultrasonic velocity and damage coeffi- 4.2.2. Computed tomography (CT) technique
cient. Therefore, the damage degree of asphalt mixture can be X-ray CT is an effective nondestructive technique for capturing
obtained. Chang et al. [94] used acoustic emission to locate the the details of a material’s internal structure. CT technique was used
starting point of the fracture in the material and analyzed the by Garcia et al. to visualize asphalt healing [45]. CT study shows
received acoustic signal to characterize the nature of the events that two sides of the crack are in contact state in the initial state,
occurring inside the sample. The rate of healing in the asphalt film and the healing part grows from the contact point. During healing,
can be quantified via ultrasonic wave transmission. The decrease of the contact point increases gradually, and the crack area decreases
signal amplitude directly reflects film damage; by contrast, if the (Fig. 13). In all the pictures, healing is stronger at the bottom of the
signal intensity increases, then the healing process may occur specimen. This phenomenon occurred, because the static pressure
[95]. The ultrasound technique is also used to monitor cracks in these areas is high. When the upper part of the specimen has not
[96]. The crack depth (z) following each interval of microwave been restored, the bottom area of the specimen will heal
treatment is expressed according to the specific energy (E/m). completely.
The ultrasound detection results show a declining ratio between The healing process can be monitored according to the changes
the crack depth and the applied E/m, indicating that the healing in cracks and voids. To reflect the healing process, air voids with a
begins at the crack tip, and the opening at the crack tip become volume above 3 mm3 are highlighted. The air voids accounted for
smaller, which diffuses to the surface until the self-healing is com- 3,755.36 mm3 in the mixture before healing and change to
pleted. The ultrasonic measurement of crack depth after each step- 1,882.11 mm3 in the mixture after healing [67]. The distribution
by-step repair interval can evaluate the depth evolution after the of air voids is uniform in the vertical direction after induction heat-
increase of repair time and verify the effect of self-healing ing. The homogeneity of healing increases when induction heating
technique. is used.

13
B. Liang et al.
Fig. 13. CT scan images of a beam during healing [45].
4.3. Summary
Performance test is mainly used to evaluate the self-healing
capacity of asphalt or asphalt mixture. However, most of the exist-
ing evalaution indexes for healing lack physical meaning and can
hardly predict the time-dependent healing process under different
conditions. New evaluation methods based on energy induction
technology, such as CT, are important directions for future devel-
opment. In addition, most of the test indicators are only realized
in the laboratory, and their applications in the road self-healing
performance evaluation require further study. The above
researches provide basic ideas for the self-healing mechanism of
asphalt and asphalt mixtures. However, improving the self-
healing ability of them is still a challenging task. The relationships
between the healing evaluation indexes for asphalt and asphalt
mixture should be established based on chemical and mechanical
analyses. Comprehensive models for predicting the degree of
self-healing and multiple self-healing of asphalt and mixtures are
also needed.
5. Improvement methods of self-healing efficiency
Self-healing is the ability of a material to repair damages auto-
matically and autonomously, which is triggered under various
methods. The increase in healing efficiency involves an active
self-healing mechanism related to the use of asphalt binder with
a high self-healing capability and a passive self-healing mechanism
related to the supplement of energy and substance. The develop-
ment trend of materials and technologies in enhancing self-
healing efficiency is shown in Fig. 14.
5.1. Materials and methods
5.1.1. Modifier
Polymer modified asphalt can form the network structure,
improve the performance of asphalt material and the ability of
binding with mineral aggregate, and improve the durability of
asphalt pavement. SBS is a widely used polymeric modifier [100-
104]. Its elastic recovery plays an important role in the self-
14
Construction and Building Materials 266 (2021) 120453
healing process of asphalt [105]. The activation energy of base
asphalt is 3.10 kJ/mol, which is slightly lower than that of SBS-
modified asphalt (5.95 kJ/mol). The pre-exponential factor of SBS
modified asphalt is 3.74 E  5 cm2/s, which is larger than that of
base asphalt (1.08 E  5 cm2/s). SBS-modified asphalt has stronger
instantaneous healing ability than base asphalt but has a higher
activation energy barrier. When the temperature is higher thanT g ,
the self-healing ability of SBS-modified asphalt increases [42]. Lv
et al. [74] investigated the effect of SBS modifier on the healing
potential of base bitumen via BBS and CT scan tests. The specimen
is submerged in a 25 °C water bath for 24 h to restore its strength.
Polymer networks in the asphalt are swollen, because saturates
and aromatics are partially absorbed into the polymer. The other
parts of high concentration of AS (highly interactive) are left intact.
SBS-modified asphalt has higher viscosity than base asphalt. The
test results show that asphalt with high AS concentration has low
flow and healing ability [51].
SBS molecules are stable at 0–40 °C, indicating that phase
change or physical chemical reaction will not occur when SBS
molecules act as fillers in the asphalt systems. Elastic polymer net-
works act as confinements and cannot repair themselves during
healing. Broken SBS molecules also cause difficulties for wetting
and interdiffusion during healing [106]. These results explain that
temperature plays a crucial role in the self-healing process of
polymer-modified asphalt.
The fracture strength, toughness, and stretchability of elas-
tomers can be adjusted by controlling the cross-linking density
of the network. Supramolecular elastomers with low T g polymer
chains and weak dynamic bonds, such as H bonds, metal–ligand
coordination, and ionic bonds, are designed to achieve autonomous
self-healing at room temperature. Unlike most self-healing materi-
als, supramolecular elastomers do not require any external stimu-
lus. When the supramolecular elastomer is cut into two pieces,
cross-linked weak dynamic bonds prefer to rupture first. Due to
the reformation of the weak dynamic bonds and the self-
diffusion of the flexible polymer chains, self-healing occurs after
contact with the cut surface [107].
Ionomers are copolymers polymers containing less than 15 mol
% ionic groups along the polymer backbone [108]. The ionic bonds
in the polymers help improve the self-healing efficiency. Ionomer
B. Liang et al.
Fig. 14. Diagram of the development trend of materials and technologies in enhancing self-healing efficiency [10,30,31,97-99].
is a kind of nanophase-separated polymer. The physical cross-
linking of ionic clusters can provide the network structure of
polymer-modified asphalt similar to that of SBS-modified asphalt.
The attraction of ionomers is a self-healing phenomenon produced
by unique ionic bonds. [109,110].
Shi et al. [109] studied the ionomer-modified asphalt of ethy-
lene and methacrylic acid system, which exhibits much better dis-
persion and smaller phase separation than polyethylene-modified
asphalt. Ionomer-modified asphalt shows better high- and low-
temperature performances than base asphalt. The initial G*/sind
values of ionomer-modified asphalt of the original, RTFO, and
PAV are 1.905, 4.41, and 3,617 kPa, while those for base asphalt
are 1.320, 3.457, and 3,401 kPa, respectively. The stiffness of
ionomer-modified asphalt at  12 ℃ is 121 MPa, and the creep rate
is 0.337, while those for base asphalt were 267 MPa and 0.317,
respectively. Ionomer improves asphalt elasticity but consumes a
long period of time to mix the ionomer into the asphalt.
5.1.2. Rejuvenator
Rejuvenators are composed of lubricating and extender oils
containing a high proportion of maltene constituents [111,112],
which can reconstitute the asphalt binder’s chemical composition
and generally be used in pavement maintenance [113]. Rejuvena-
tors used in asphalt pavements should meet five essential condi-
tions, as follows: (1) good compatibility with bitumen, (2) high
temperature stability, (3) ability to survive mixing and construc-
tion conditions, (4) healing temperature ranging from 30  40 °C,
and (5) continuous/multi-time healing ability.
5.1.3. Filler
Conductive fibers are placed in asphalt mixtures and then
heated by induction devices to promote self-healing [114,115].
The steel wool to porous asphalt can be heated quickly with an
15
Construction and Building Materials 266 (2021) 120453
induction generator, and the microcracks in the material can be
closed by high-temperature healing of the bitumen via induction
heating, thereby prolonging the fatigue life. At the same time, steel
wool improves the particle resistance, indirect tensile strength, and
fatigue resistance of porous asphalt, thus delaying the spalling of
pavement and prolonging the fatigue life of pavement [90]. The
effect of Ni  Zn ferrite powder on the self-healing efficiency of
asphalt mixture was also investigated [61]. The fatigue life exten-
sion ratio of 80% (volume fraction of mineral powders) ferrite-filled
asphalt mixture with a 50% damage can reach 1.33 after 3 h of
healing at 55 °C by using a microwave.
Metal shavings, which are waste materials from the metal
industry, are added to the asphalt mixture to facilitate self-
healing via microwave heating [116]. The average healing ratios
of the mixtures with and without metal shavings are 0.5374 and
0.4526, respectively, thereby exhibiting potential in developing
environmentally sustainable asphalt pavement.
5.2. Enhanced technology
5.2.1. Electromagnetic induction
Indirect heating mechanisms are tailored depending on antenna
materials and energy sources, such as electromagnetic and
mechanochemical activation [117]. Electromagnetic induction
method has been applied for the self-healing properties of compos-
ites. Under the action of electromagnetic induction, the crack is
closed via molecular diffusion because of the thermal effect of con-
ductive materials and rest time.
The scheme of the induction heating system behavior is shown
in Fig. 15 (a). Micro cracks were observed in the asphalt. Sufficient
volume of conductive fibers or fillers form a closed-loop circuit
around the microcrack. If the magnetic induction and conductive
materials are placed near the coil, eddy current will be generated
B. Liang et al.
Fig. 15. Electromagnetic induction heating. (a) Closed cracks through induction
heating [118] and (b) fatigue life extension caused by multiple instances of
induction healing [90].
in the closed loop circuit with the same magnetic field frequency.
When the eddy current acts on the resistance of the material to
generate heat, the asphalt melts, and the cracks are closed
[118,119]. Fig. 15 (b) shows the fatigue life extension induced by
natural and induction heating. The original fatigue life of the sam-
ple containing 1.27% steel wool is 95,700 cycles. With the rest peri-
ods alone, the fatigue life under natural healing is 149,860 cycles
with a fatigue life extension ratio of 56.7%. Considering four
instances of damage loading of 50,000 cycles followed by 4
instances of induced heating and rest period, the fatigue life is
extended to 277,720 cycles, which is 2.9-fold higher than that of
the original fatigue life with a fatigue life extension ratio of 190%.
In addition to the fiber content, the self-healing effect is affected
by the temperature. Dai et al. [88] evaluated the healing ability by
heating the surrounding cement material via energy induction.
Fracture-healing tests are conducted using three samples at differ-
ent heating temperatures. At 60 °C, different samples show 35.8%
and 56.8% recovery of peak loads after nine cycles. Exactly 63.2%
and 73.6% of the original fracture strength were obtained at the
same condition at 100 °C. When heating temperature was 100 °C,
the best healing effect was achieved without affecting the physical
properties of asphalt materials.
5.2.2. Microwave induction
Microwave heating is also a typical technique used to promote
self-healing. Gallego et al. [120,121] introduced steel wool and gra-
phite additives into the mixture to increase their susceptibility to
electromagnetic induction. Results showed that the power con-
sumption of microwave devices is much lower than that required
to produce similar effects via electromagnetic induction. The effect
16
Construction and Building Materials 266 (2021) 120453
of 0.2% medium steel wool in microwave-heated mixture is similar
to that in 1.5%5% steel fiber in an electromagnetic induction mix-
ture, which corresponds to significant savings. A. Gonzalez et al.
[116] compared the heating effect of microwave and induction.
The average surface temperature of the asphalt samples after
microwave heating was 71.7 °C, while the temperature achieved
via induction heating was 50.85 °C,
The temperature of microwave heating is difficult to control; it
may be higher than the flash point temperature of asphalt and
destroy the chemical structure of binder. Therefore, heating time
should be strictly controlled [99]. The optimum microwave heating
time is obtained at the highest healing levels without an early
damage of the bitumen.
5.2.3. Encapsulation technology
5.2.3.1. Microcapsules. The addition of self-healing microcapsules
into the asphalt binder is another effective way to autonomously
repair the microcracks in asphalt concrete and further enlarge
the fatigue life. This particular approach involves thw incorpora-
tion of a microencapsulated healing agent and a dispersed catalyst
within a polymer matrix [122-125]. Once cracking occurs, the
microcapsules are ruptured by the propagating crack fronts and
release healing agent into the cracks via capillary action [126].
The self-healing mechanism of microcapsules is shown in
Fig. 16. The extension of the cracks causes the microcapsules to
rupture due to tip stress and release the renewable agents, which
fill the cracks through wetting and spreading. The regenerator
flows out of the microcapsules and fills cracks and fuses with the
asphalt to regain the properties of the original material.
The rejuvenator’s diffusion is the key factor in the microcapsule
repair technology. Diffusion rate and depth remarkably affect the
self-healing rate. Fig. 17 (a) shows the process of microencapsu-
lated rejuvenator diffusion into bitumen. Microcrack was gener-
ated because of the low-temperature brittleness. Rejuvenator
diffusion into bitumen was monitored continuously via the modi-
fied FTIR-ATR method. The diffusion coefficient was obtained by
quantifying the change in absorbance as wave numbers. The diffus-
ing substances are flushed over the film with a steady concentra-
tion at the film surface. Fig. 17 (b) illustrates the microcrack
generation process through a self-designed installation. The appli-
cation was accomplished by gluing brass frames on top of the
prism. The bottom layer (the bitumen) was allowed to settle in
the heated sample holder at 100 °C for 30 min to obtain absolute
contact between the sample and prism and to avoid initial prob-
lems with air bubbles and other types of distress at the beginning
of the diffusion test. All thin bitumen layers had a thickness of
2 mm. The temperature was set and infrared absorbance recorded.
In 2010, Garcia et al. [127] studied whether capsules must resist
high temperatures during mixing, transportation, and placing, a
common process temperature in asphalt concrete. The thermal sta-
bility of the capsules was investigated by tracking the mass loss of
the capsules at different isotherm temperatures for 2 h each. The
mass loss was only approximately 3%.
Sunflower oil was chosen to replace the aromatic oil, because it
is less harmful to human health and the environment [128]. Only
very small mass losses happen after heating the capsules. These
results proved that approximately 45% of the total cracking dam-
age disappears during the resting period. The diameter of the cap-
sule was designed according to the amount of oil required for the
self-healing of the asphalt mixture. In 2016, Garcia et al. investi-
gated the effect of microcapsule size [129]. Five kinds of capsules
with different diameters were prepared, and their mechanical
strength and composition were characterized. The mixing proper-
ties and compactness of capsules in the asphalt mixture were stud-
ied, and the effects of capsules on indirect tensile strength,
modulus, and fatigue life of asphalt mixture specimens were quan-
B. Liang et al.
Fig. 16. Illustration of multi-self-healing ability for microcapsule/bitumen composite. (a) Schematic of the microcapsule/bitumen composite; (b) Microcrack generation; (c) A
microcrack broken following the diffusion area; (d) Closed crack; and (e–f) Schematic of molecular diffusion during crack closure.
tified. Large capsules contain a large amount of oil, but they are not
as strong as small capsules. The diameter of the capsule must be
selected in accordance with the amount of oil required for self-
healing of the asphalt mixture.
The physicochemical properties of novel microcapsules con-
taining rejuvenator via the in situ polymerization of MMF prepoly-
mer are synthesized and characterized. A two-step coacervation
method was successfully applied to enhance the thermal stability
and compatibility of shells with styrene maleic anhydride as the
surfactant [131]. TGA tests indicated that the thermal decomposi-
tion temperature of microcapsules is higher than the melting tem-
perature of asphalt. Three typical functional groups (i.e., phenolic,
anhydride, and carboxylic acid) in bitumen can undergo dehydra-
tion or esterification reactions with the MMF resin. These reactions
can result in the formation of chemical bonds between the shells
and bitumen, which will enhance the interface stability in endur-
ing heat treatment and bearing stress. The process of repairing
cracks by using microcapsules on the basis of capillary phe-
nomenon and diffusion behavior was also explained after verifying
the stability of the microcapsules [132]. Results showed that reju-
venator filled cracks with the aid of capillarity at a movement
speed based on the volume of microcapsules in bitumen. After-
ward, the thermal, mechanical, and interface stability of the micro-
capsules in bitumen were further studied [133]. Microcracks fairly
penetrate the interphase of shells, and the rejuvenator outflows the
shells.
The microcapsules with DMP or SBS/DMP as core and urea/
formaldehyde resin as shell were prepared successfully [134].
17
Construction and Building Materials 266 (2021) 120453
The bitumen containing DMP microcapsules requires seven days
of rest time to restore the original strength, but only three days
are necessary to restore the original strength for asphalt containing
SBS/DMP microcapsules. Sharareh et al. [89] investigated the ther-
mal stability of microcapsules with sunflower oil as the core mate-
rial and evaluated the effect of the microcapsule in increasing the
self-healing ability of asphalt mixtures. Asphalt binder stiffness
and m-value measurements demonstrated that the microcapsules
decreased the low-temperature stiffness and increased the m-
value of the binder blends. Crack healing, as defined by the reversal
of the crack opening, was validated in all mixtures via digital image
analysis. Sunflower oil, as a rejuvenator, showed the best perfor-
mance in terms of self-healing efficiency. The difference in healing
efficiency (room temperature vs. oven temperature) was the lar-
gest at the first day, which became less pronounced with the pro-
gression of healing. Double-wall polyurethane and urea–
formaldehyde can withstand the temperature range of the whole
mixed production. The microcapsules containing SBS/DMP showed
good performance, and their self-healing behavior and stiffness
could reach 1.7 times of their initial values.
In summary, the microcapsules containing rejuvenator may
allow the realization of smart pavements. Table 3 summarizes
the material design of microcapsules.
5.2.3.2. Hollow fiber. The possibility of filling cracks of the small
spherical microcapsules is limited due to the small dosage of heal-
ing agent per capsule. A large number of microcapsules in asphalt
mixture reduces the quality of pavement and leads to premature
B. Liang et al. Construction and Building Materials 266 (2021) 120453

containing rejuvenator for bitumen were fabricated via a spinning

Fig. 17. Diffusion process monitoring. (a) Illustration of the diffusion process of the
microencapsulated rejuvenator into bitumen; (b) Illustration of FTIR–ATR method
to test the diffusion behavior of rejuvenator in bitumen; [130].
road destruction. Inspired by bionics, hollow fiber containing heal-
ing agents has been applied as materials to heal cracks in bitumen,
as shown in Fig. 18 (a) and (b). The ruptured biomimetic capillaries
can self-heal with the aid of blood stream. Fig. 18 (c) illustrates
self-healing bitumen by using biomimetic capillary hollow fibers.
A good long-distance supply of healing agents is obtained by stor-
ing the healing agent in long, hollow fibers [141-143]. Dry and Sot-
tos et al. [144,145] pioneered the concept of releasing healing
chemicals stored in hollow fibers to repair damage. Biomimetic
capillary hollow fibers containing rejuvenator for self-healing
asphalt was reported by Su et al. [146]. Self-healing hollow fibers
method with PVDF as fiber material. Microcapsules survived in
bitumen, which resisted high temperature and strong agitation
without premature damage. The fibers survived in hot bitumen
without break with a good thermal stability. The fibers were
reputed by the crack in bitumen and rejuvenator flowed outside
of fibers. A spinning technology was used to make self-heating hol-
low fibers containing a rejuvenation agent to overcome low
mechanical properties and degradation. The results indicate that
the hollow fiber containing rejuvenator can enhance the self-
healing capability of aged bitumen. Future works will optimize
the microstructure of fiber/bitumen composites and investigate
the micromechanical properties of self-healing behaviors.
Sodium alginate was selected as the encapsulation material due
to its advantages of low cost, organic, low environmental impact,
and self-degradation [97]. Alginate fibers have excellent potential
as self-healing materials for asphalt pavements. They can be
inserted into bituminous mastic and increase the strength of
asphalt mixes by 36%. Several environmental SEM images of com-
partmented fibers are shown in Fig. 18 (d–f). The rejuvenator was
distributed along the fiber axis.
The fiber is effective for the healing of microcracks, but the
effect of the system on the healing of large cracks is not as good
as that of microcracks, because only a small amount of rejuvenator
is encapsulated in the fibers. Amir et al. [98] further optimized the
design of a compartmented alginate fiber encapsulating rejuvena-
tor. The maximum number of rejuvenator can be optimized to
improve the system’s healing efficiency without damaging its ther-
mal and mechanical properties. Fig. 18 (g) shows that the optimum
fiber content in the asphalt mix is 5% for the compartmented fibers
with a rejuvenator/alginate ratio of 70:30.
5.2.4. Nanoparticle reinforcement
Asphalt modification at the molecular level is the best choice for
developing asphalt mixture with strong self-healing ability [77].
The use of nanoparticle-modified polymer materials is an emerging
and interesting approach in creating self-healing materials to
repair cracks, which does not involve the destruction and rebond-
ing polymer chains but involves a dispersed particulate phase to fill
cracks and flaws if crack occurs (Fig. 19). The interaction between
nanoparticles and polymers is minimized by the segregation of
nanoparticles in the crack and pre-crack regions [147,148].
Lee et al. [149] constructed a polymer/nanoparticle composite, a
self-healing system that actively responds to the damage and may
heal itself for multiple times. The modeling results reported by
Tyagi et al. [150] indicated that nanoparticles may move toward
the damaged area via a polymer-induced depletion attraction. An

Table 3
Material design of the microcapsules.

Core Shell Performance References

Porous and. aromatic oil Epoxy resin, cement Resist high temperatures and stresses [127]
Porous and sunflower oil Particles of cement type I 52.5R bonded by liquid epoxy resin Resist mechanical forces [128]
Porous and sunflower oil Particles of cement type I 52.5R bonded by liquid epoxy resin Not affect the fatigue resistance [129]
Dense aromatic oil Commercial prepolymer of melamine–formaldehyde modified Easily dispersed [135]
by methanol
Dense aromatic oil Commercial prepolymer of melamine–formaldehyde modified Large plastic deformation without [133]
by methanol breaks
DMP or SBS/DMP Urea/formaldehyde resin Restored strength for 7 or 3 days [134]
Composite rejuvenation Urea/formaldehyde resin Healing efficiency of 38.67% [136]
Lubricating and extender oils Melamine–formaldehyde resin 2:1 and 1:1 core/shell thickness ratio [137]
Sunflower oil was encapsulated in calcium- Epoxy/cement composite Large reductions in cracks [138]
alginate
Sunflower oil and PennzSuppress Polyurethane and urea-form aldehyde Reverse aging [139]
Sunflower oil Polyurethane and urea-form aldehyde Recovering 1.7-fold of its initial stiffness [89]
Rejuvenator Melamine–urea–formaldehyde Enhanced fatigue life of aged asphalt [140]
enhanced

18
B. Liang et al. Construction and Building Materials 266 (2021) 120453

Fig. 18. Illustration of self-healing bitumen by using biomimetic capillary hollow fibers. (a) Biomimetic capillaries; (b) rupture of a biomimetic capillary; (c) self-healing
asphalt by using hollow fibers containing rejuvenator [146]; (d) general view of a fiber; (e) dimeter of the cross-section of the fiber; (f) longitudinal cross-section of the fiber
[97], and (g) effect of fibers on asphalt mix stiffness [98].

obvious stress concentration may be observed at the tip of the sur-
face notch, which will eventually lead to the propagation of cracks
in the system and the degradation of mechanical behavior. The
morphology obtained from the MD simulation serves as the input
to the lattice spring model, which determines the mechanical
properties of the nanocomposite-coated surface. The application
of such nanocomposite coatings could yield defect-free surfaces
with enhanced mechanical properties. The morphology simulated
by MD was used as the input of the lattice spring model, which
determines the mechanical properties of the nanocomposite coat-
ing surface. The application of this nanocomposite coating may
produce a defect-free surface and enhance the mechanical
properties.
Some aspects of the computer simulation have been verified by
experiments. Gupta et al. [16] have demonstrated the migration
and clustering of embedded nanoparticles around the cracks in a

19
B. Liang et al. Construction and Building Materials 266 (2021) 120453

multilayered composite structure. Cross-TEM analyses revealed

that the nanoparticles are uniformly and preferentially segregated
at the interfaces of matrix and additive layer. Fluorescence micro-
scope images show that nanoparticles migrate and accumulate on
the surface of the crack. The migration of nanoparticles depends on
the enthalpy and entropic interactions between the matrix and the
nanoparticles.
To understand the characteristics of nanomaterials in asphalts,
researchers have used nanomaterials in many applications to
improve the fatigue [151,152], rheological [153,154], and aging
properties of asphalt [155,156]. The effectiveness of nanoparticles
depends highly on the physicochemical properties of base compo-
nents, which strongly influence the morphological configuration
within the bituminous media [157].
The asphalt mixed with carbon nanotubes (AT) and nanoclay
(AC) illustrates that high S/Ar content will result in a good self-
healing property. The increase saturates-to-aromatics ratio (S/Ar)
will improve self-healing capabilities, which may explain the
above results. The S/Ar value of A bitumen was obviously higher
than that of B bitumen, indicating that the moleculat structure of
A asphalt is longer and thinner, and the content of branched-
chain decreased. Therefore, the molecules will diffuse faster, and
A asphalt binder will tend to heal the microcracks more rapidly.
Asphalt mixture B with high aromatics content showed different
Fig. 19. Schematic of nanoparticle movement during crack growth in thermoplas- results, as shown in Fig. 20 (a) (b).
tics [30].
In 2017, Amin et al. [158] enhanced the self-healing properties
of asphalt mixtures by adding spherical nanosilica with small size

 0 
 
   analysis of base asphalt and (b) theoretical maximum gain in mechanical properties (DG1 ) versus the degree of
Fig. 20. Effect of nanoparticles on self-healing. (a) Chemical
damage experienced at the onset of rest periods (DGLOSS ) [157].

20
B. Liang et al.
and high density (2.33 g/cm3). The self-healing index reached
88.7% when the nanosilica content reached 3%. Nanosilica
enhances the randomness of surface molecules and accelerates
molecular diffusion, thereby promoting the rapid healing of micro-
cracks. Researchers have established a means to tailor the macro-
scopic behavior of the composite by harnessing both enthalpic
and entropic interactions to control the nanoparticle distribution
in the polymer matrix. The combination of nanoparticles and poly-
mers enables the tailoring of the composite’s macroscopic behav-
ior, which is related to mechanical damage due to the transport
and filling effect of nanoparticles toward the damaged sites to
address the sustainability issues [16].
5.3. Summary
Microcapsules containing regenerant have been widely studied,
but their mechanical properties and the effective combination of
regenerant and original asphalt remain unclear. The effects of a
modifier are greatly affected by the type of materials and the
chemical composition of matrix asphalt, which needs further anal-
ysis. Nano material agglomeration in bitumen weakens or even
negates the role of nano materials. The damage of interface
between nanoparticles and asphalt may also lead to a change in
the asphalt performance. Therefore, the healing mechanism of
nano asphalt needs further discussion. Induction therapy for field
applications is mainly limited by fact that fibers are difficult to
mix, and the heating time is excessively long. In future studies,
the fibers must be replaced by metal aggregates to allow for fast
mixing and heating.
The temperature increment after induction heating is limited
because the temperature rapidly reverts back to the rest level.
The upper part of sample after induction heating has higher tem-
perature than the lower part. Most existing evaluation indexes
for healing lack physical meaning and can hardly predict this
time-dependent process under different conditions. In the future,
material sustainability and reduced energy costs must be
considered.
6. Conclusions and prospect
The self-healing mechanism of asphalt materials and the rela-
tionship between the self-healing ability and asphalt fatigue life
at the molecular level for an improved pavement performance is
summarized. The factors affecting the self-healing rate, the test
methods for evaluating the self-healing performance, and the tech-
niques for improving the self-healing efficiency of asphalt were
discussed. Considering all the factors, we draw the following
conclusions:
(a) Molecular diffusion plays an important role in the self-
healing process of asphalt, and the increase of diffusion coefficient
accelerates its self-healing performance. By using polymers and
nanomaterials to change the chemical composition of asphalt or
by using other techniques that provide similar properties, inter-
molecular forces are enhanced, self-healing efficiency is improved,
and its original properties are restored.
(b) The influence of asphalt molecular structure and the change
of asphalt composition is analyzed in detail. S/Ar, CH2/CH3, HA,
time, and temperature enhanced the self-healing efficiency. At
the same time, the aromatic structure, aging, damage, and mois-
ture of MMHC had negative effects on self-healing efficiency. Con-
trolling the healing temperature is the key factor to reach the
optimal healing level.
(c) Energy-based evaluation method and the application of new
technologies are the future development direction. The healing
ability of asphalt binder is defined as the activation energy. The
21
Construction and Building Materials 266 (2021) 120453
energy consumption of electromagnetic and microwave induction
technologies, the combination of microcapsule reinforcer with
original asphalt, and the availability and economy of modified
materials need to be further studied.
Research on self-healing of asphalt materials is important in
developing sustainable roads. Understanding the self-healing
mechanism, influencing factors, assessment techniques, and
improvement aspects for asphalt materials and the relationship
between its self-healing ability and fatigue life can aid in enhanc-
ing the preventive maintenance and performance of asphalt pave-
ment. This paper provides an important reference for the
development of asphalt pavement self-healing technology.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgements
This work was supported by the National Natural Science Foun-
dation of China (Grant No. 51778071) and the Open Fund of State
Engineering Laboratory of Highway Maintenance Technology at
Changsha University of Science & Technology (Grant No.
kfj150101).
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