Journal of Industrial and Engineering Chemistry 29 (2015) 330–337

Contents lists available at ScienceDirect

Journal of Industrial and Engineering Chemistry

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

Preparation and characterization of microcapsule-containing

self-healing asphalt
Kyungho Chung a, Seunghyun Lee a, Moonsoo Park a, Pyeongjun Yoo b, Youngkeun Hong a,*
a
Department of Polymer Engineering, The University of Suwon, Hwasung-si 445-743, Republic of Korea
b
Highway Research Division, Korea Institute of Construction Technology, Goyang-si 411-712, Republic of Korea

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

Article history: Microcapsules-loaded with healing agent were successfully prepared in which dimethylphenol(DMP) or
Received 6 February 2015 SBS/DMP forms core while urea/formaldehyde resin constitutes shell of the microcapsule. Microcapsule-
Received in revised form 15 April 2015 containing asphalts displayed better mechanical properties than non-contained ones. The impact
Accepted 18 April 2015
strength of microcapsule-containing asphalts improved over time. Microcapsule(DMP)-containing
Available online 24 April 2015
asphalt needed 7 days of rest time to restore its original strength, but it took only 3 days for
microcapsule(SBS/DMP)-containing asphalt. This tells that microcapsule(DMP or SBS/DMP) containing
Keywords:
asphalt posses excellent self-healing potential. SEM and X-ray photos illustrate that DMP on the asphalt
Asphalt binder
fracture surface, which burst out of the microcapsules when cracks occur on the surface of the asphalt,
Microcapsule
Healing agent undergoes polymerization to poly(phenylene oxide), filling cracks and healing damage.
Self-healing ß 2015 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights
Impact strength reserved.

Introduction Self-healing mechanism can be categorized into three classes:

Generally asphalt cracks easily at temperatures around 208 C and
around 608 C rutting(plastic deformation) occurs. Modifying asphalt
means strengthening its physical properties in order to allow plastic
deformation to occur at temperature higher than 608 C, and prevent
asphalt from cracking too easily at low temperatures [1].
Although modified asphalt has greater durability compared to
the straight asphalt, it still has limited lifespan. Minute cracks
develop into potholes, disrupting comfortable driving, which is why
necessity for self-healing asphalt has been the subject of research as
it can retain sustained road surface for an extended period of time.
Self-healing material is a type of smart material that can heal
damages resulting from use for a prolonged and return to its
original form [2]. It originates from the fact that organisms heal
themselves when they get injured. When a material cracks or is
damaged, its physical properties change and can lead to
breakdown of the material. Generally cracks can be repaired
easily by hands, but minute cracks are usually too small to detect. If
a material has the ability to repair small damages, it will reduce
repair costs and production cost as well since the material will last
longer, ultimately reducing CO2 production.
* Corresponding author. Tel.: +82 31 220 2487; fax: +82 31 220 2529.
E-mail address: ykhong@suwon.ac.kr (Y. Hong).
physical, thermal, and chemical mechanism. The physical
mechanism can be subdivided into two types. In one type,
nanopowder like montmorillonite are mixed with thermoplastic
material [3–5]. When the material cracks or breaks, nanoparticles
are getting close to each other since the medium is depleted and
fill the cracks by crowding the empty space owing to polymer-
induced depletion particle attraction [6]. In the other method,
healing agent-contained microcapsules or glass tubes are mixed
with the material [7–9]. This healing agent flows out when the
material cracks and fills the empty space. Self-healing material using
microcapsules is prepared by forming the microcapsule containing
healing agent inside and by mixing them with matrix material.
When material starts to crack, microcapsules on the crack
propagation path are also destroyed, and healing material in the
capsule leaks out filling the cracked hole. When the cracking of
matrix occurred, monomer flows out from the microcapsules and is
polymerized by the catalysts that exist in the cracked area. This
polymer fills the crack area and repairs the matrix restoring its
original form up to 80% on the basis of fracture strength. White [8]
used dicyclopentadiene as healing agent and bis(tricyclohexylpho-
sphine)benzylidine ruthenium dichloride(Grubbs catalyst) as cata-
lyst. Using the ring-opening metathesis polymerization technique,
White was able to self-heal the cracks in the thermoset material.
Other self-healing materials using microcapsules were tested by Cho
[9]. Here healing material was a mixture of polydimethylsiloxane

http://dx.doi.org/10.1016/j.jiec.2015.04.011
1226-086X/ß 2015 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337
and polydiethoxysiloxane with hydroxyl end group and the catalyst
was di-n-butyltin dilaurate that healed microcracks on metal
surface by condensation polymerization.
In the thermal mechanism, matrix contains compounds which
use Diels–Alder reaction for polymerization or conductive
materials such as carbon fiber and the matrix can be healed when
heat is applied [10–12]. Furan molecules containing double bonds
react upon heating (808 C) to give a network polymer, i.e., self-
healing polymer, via Diels–Alder reaction [10]. More recently
White [13] used a vascular (i.e., glass tubes) synthetic system to
restore mechanical functions by shape reforming (i.e., filling up the
crack) microcracks (d > 35 mm) with gelation within 20 min and
by solidifying the gel through polymerization within 3 h.
In the chemical mechanism, cracks can be sealed by attraction
of each side of the crack where the attraction force is one of the
secondary valence forces (dipole interaction, hydrogen bond, ionic
bond) [14–16]. Leibler [14] developed a self-healing rubber using
supramolecule. Small molecules extracted from vegetable oil form
3-dimensional supramolecular structure by hydrogen bonding. In
this case, hydrogen serves as an adhesive between atoms. When
rubber is cut, unpaired hydrogen atoms are exposed at the
intersection. If the cut surfaces are put back together, hydrogen
bonds form again in 10 min and the material self-heals. After this
healing process, the rubber maintains its original property that it
stretches up to 4 times its original length. Even after being cut and
reattached several times rubber maintains its characteristics as
long as it is reattached within 12 h.
Asphalt is one of the most common types of pavement materials
used in the world. It is a composite material that consists of a
mixture of asphalt binder and aggregates. This material must resist
all traffic loads in good conditions under many different climatic
conditions for a long time. In order to maintain these character-
istics during its lifetime, asphalt’s wearing courses should be
constantly maintained and repaired. Little cracking on a road can
mean the start of large distress.
Recently, a number of researchers have demonstrated phenom-
enologically that asphalt mixtures have the capability to heal
cracks [17–20]. They have shown that when given a certain
amount of rest time, the modulus of asphalt mixtures can have
some increase after the rest time and the overall life can be
increased. These studies have led to a new way of describing the
performance of asphalt materials: asphalts are healable.
As a complex composite material, asphalt mixture consists of
two major components: asphalt binder and aggregates. Kim [19]
and Song [21] proposed that in asphalt mixtures two types of
healing exist: adhesive healing at the asphalt-aggregate interface
due to the rebonding of the asphalt to the aggregates and cohesive
healing within the viscoelastic asphalt binder due to the cross-
linking of asphalt at the crack surface.
By far, three approaches to realize self-healing asphalt exist: the
first one is that compounds are incorporated into asphalt binder to
increase strength and repair bond. Lee [22] and Pang [23] found
that SBS positively affect the self-healing of asphalt. Little [31]
explored the possibile effect of hydrated lime on healing ability of
asphalt. Hydrated lime—added asphalt when it has a high
asphaltene content showed healing ability. The second one is
that embedded encapsulated chemicals are used in asphalt binder
to decrease stiffness and repair bond. Microcapsules filled with
maltene are mixed with asphalt mixture [24]. When a crack
appears in the pavement close to a microcapsule, it would be
broken and the maltenes will be in contact with the asphalt
around. It will rejuvenate the asphalt and enhance self-healing. In
another study [25], embedded microcapsules containing rejuve-
nator were prepared, and healing capability was validated with
tests. The third one is that local heating inside the asphalt with
induction energy is used to repair the binder and to improve the
331
properties again [26,27]. Steel wool was added to asphalt mixtures.
The steel wool heated by induction energy melts the asphalt that
flows into the microcrack and fixes the aggregates back to
pavement surface. Thus the system reduces raveling. A problem
of this system is that it requires human intervention to complete
the healing process.
It is proposed that the healing of asphalt is a three step process
[28,29]: (1) wetting of the faces of a crack, (2) diffusion, caused by
Brownian motion, driving the molecules to the low-energy region
near the crack, and (3) randomization of the diffused molecules to
attempt to reach the original strength of the material.
Polyphenylene oxide(PPO), one of the engineering plastics, can be
manufactured by polymerization of 2,6-dimethylphenol(DMP)
through oxidation reaction of oxygen molecules using cuprous
chloride as the main catalyst and pyridine or di-t-butylethylenedia-
mine as cocatalyst [30]. DMP also self polymerizes into PPO in asphalt
by the components of asphalt, vanadiums and amine compound [31].
In this study, monomer DMP and SBS(styrene–butadiene–
styrene triblock copolymer) rubber were used as healing agent.
They were used as core material in producing microcapsules and
incorporated into manufacturing self-healing asphalt. It was
hypothesized that DMP will polymerize into PPO by metals in
asphalt and by oxygen molecules in the air and this will seal the
crack and consequently heal the material.
Experimental
Materials
Urea and formaldehyde to prepare urea(U)/formaldehyde(F)
resin, which forms the shell of microcapsules, were purchased
from Samchun Chemical. 2.6-DMP and SBS(KTR101, linear type),
which constitutes the core of the microcapsules, were obtained
from Aldrich and Kumho Petrochemical, respectively. Triethyle-
netetramine(TETA) which can liquify DMP and SBS to be used as
core solution of the microcapsule was purchased from Aldrich.
Polyvinylalcohol(PVA) and sodium dodecyl sulfate(SDS) which
were used as emulsifier and surfactant each for preparing
emulsions purchased from OCI and Aldrich, respectively. Asphal-
t(AP-5, penetration 60–70) was provided by SK Petrochem.
Preparation of microcapsules
For preparing the microcapsule, emulsion was first made that in
1000 ml reactor distilled water 200 ml, emulsifier PVA 2.2 g and
surfactant sodium dodecyl sulfate 0.5 g were added and thor-
oughly mixed. Prepolymer forming the shell of the microcapsule
was made that urea 3.6 g reacted with formaldehtde 0.9 g at 708 C
for 1 h in another container. TETA 2 g was used to liquify DMP 5 g
for DMP only forming the core. Thus DMP solution for the core was
obtained. For SBS and DMP both forming the core, TETA 2 g
dissolved DMP 2.5 g first and then SBS 2.5 g. Thus SBS/DMP
solution for the core was obtained.
Reactor containing the emulsion was set up in a bath and the core
solution(DMP or SBS/DMP) was added and mixed at 708 C for 30 min.
Then the prepolymer was added and stirred at 250 rpm and reacted for
3 h while adjusting pH to 3. The emulsion solution was washed and
filtered using water containing 10% methanol then separated
microcapsules were dried in a vacuum oven at 308 C for 5 h.
Yield (Ymc) of obtaining the microcapsule was calculated using
the following equation;
 
W mc
Y mc ¼  100
Wt
where Wmc is the weight of obtained microcapsule and Wt is the
weight of all agent composing shell and core of the microcapsule.
332 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337

The thermal behavior of the microcapsules was analyzed using

differential scanning calorimetry(Perkin Elmer Pyris6 DSC) in the
current of nitrogen gas.

Preparation of microcapsule-containing asphalt

Encapsuled asphalt was made that asphalt 200 g was mixed

with microcapsule 20 g in 1000 ml kettle at 1608 C for 1 h with the
stirring speed of 500 rpm.

Testing of encapsuled asphalts

Measuring the self-healing tendency of encapsuled asphalt was

conducted through Izod impact strength test of the asphalt at

Fig. 2. Optical microscopy photo of obtained microcapsules(SBS/DMP).

108 C. Test specimens were made according to ASTM D256. Seven

specimens were prepared for each composition. The test was
performed as in Fig. 1 that after original specimen was broken upon
impact test, two parts were joined in one and wait a certain period
of time at 208 C, tested again at 108 C. The test temperature of 108 C
is due to the fact that the specimen at 208 C is hardly broken.
Profile of the obtained microcapsule and the fracture surface of
specimen after impact test were observed with SEM(JEOL). Size
distribution analysis was performed using Liss microsytems
equipped with counter. The microstructure of the microcapsule
itself and microcapsule-containing asphalt were observed with X-
ray reflection diffractometer(Rigaku, XRD9D/MAX 2C) using CuK
radiation (l = 1.542 Å).

Results and discussion

Characterization of microcapsules

Microcapsules between one having core of DMP and the other

of SBS/DMP are not differentiated in microscopic view since they
both have same kind of shell, which is U/F resin. Also, yield of
producing microcapsules of both was about 43%. The micro-
capsules which have SBS/DMP solution in core are shown in Fig. 2.
It can be seen that they are all right spheres and some small ones
have their diameter of around 20–30 mm and some larger ones
have 400–600 mm. Becke lines which show wall thickness can be
observed. The thickness ranges from 16 mm to 83 mm. The average

Fig. 1. Procedure (a ! b ! c ! d) of preparing specimens for impact strength test to

measure self-healing tendency: (a) original, (b) broken (c) joining, (d) resting. Fig. 3. SEM photo of shell surface of the microcapsules(DMP).
 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337 333

Fig. 4. Size distribution of the microcapsules(DMP).

wall thickness is about 30 mm. Their surfaces are relatively smooth
(Fig. 3). Their average diameter is about 160 mm (Fig. 4).
Fig. 5 shows the DSC thermograms for DMP itself, SBS, and two
kinds of microcapsules which contain DMP or SBS/DMP in the core.
Both of microcapsules’ shell are composed of U/F resin. The
monomeric DMP existing as a solid shows a endothermic peak at
508 C. SBS shows a Tg at 1808 C, which belongs to hard block of SBS.
Both of microcapsules show a same Tg at near 908 C, which belongs
to UF resin. However microcapsules which contain SBS/DMP in the
core show another Tg at 2138 C, which belongs to the SBS. This tells
that microcapsules we obtained are composed of U/F resin and
DMP or SBS/DMP.
Characterization of encapsuled asphalts
The original impact strength of pure(or straight) asphalt and
microcapsule-containing asphalts are shown in Fig. 6. Pure asphalt
shows the impact strength of 3.91 J/m. The impact strength
of microcapsule(DMP)-containing asphalt and microcapsule
(SBS/DMP)-containing asphalt are higher than that of the pure
asphalt, which increased by 5.4% and 6.1%, respectively. It seems
that microcapsules having shell made of U/F resin act as a
reinforing filler for asphalt.
Self-healing tendency was measured by self-healing efficiency
which is calculated from the ratio of the strength upon rest periods
to the original strength. The impact strength of microcapsu-
le(DMP)-containing asphalt upon one day passed after the test
shows 89% of that of the original. On the seventh day it restores the
original strength(101%) and efficiency progressively increased
(Fig. 7). Microcapsule(SBS/DMP)-containing asphalt reveals a little
different tendency that on the first day it shows 95% efficiency
which is higher than that of microcapsule(DMP)-containing
asphalt and on the third day it restores the original strength(108%).
It seems that this is contributed from the characteristics of SBS that
it act as an elastomer and a good adhesive in between two faces of
broken specimen. However after it reaches the top(114%) on the
seventh day the self-healing efficiency reaches almost a plateau.
The pure asphalt never reached the original strength during

Fig. 5. DSC thermograms of DMP, SBS, and microcapsules containing DMP only or SBS/DMP solution in the core.
334 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337

Fig. 6. Impact strength of asphalts; (1) pure asphalt, (2) microcapsule(DMP)-containing asphalt, (3) microcapsule(SBS/DMP)-containing asphalt.

Fig. 7. Healing propensity of asphalt containing microcapsules upon the rest period: pure; pure asphalt, DMP; microcapsule(DMP)-containing asphalt, SBS + DMP;
microcapsule(SBS/DMP)-containing asphalt.

duration of the test. It started from an 85% efficiency and ended at

96%. The pure asphalt’s self-healing efficiency is allegedly
attributed to it’s adhesive nature [32].
Fig. 8 shows the healing agent in the core of the microcapsule
which was instantly and simultaneously ruptured as the impact
was given on the asphalt. This photo tells that a solution as a
healing agent is in the microcapsule.
Now the encapsuled asphalt was cut by a stationary cutter and
the side view of the crack was obtained. Fig. 9 shows the process of
crack remedy by the healant which came out of the broken
microcapsules on the surface of asphalt. The healant fill the bottom
of the crack but the quantity is very small. It must be considered
that the specimen contained microcapsule only 10 wt% of the
asphalt. If we want more prominent effect, then we need to add
more microcapsules. such as 20 or 30%.
To see whether DMP polymerized to PPO, DMP itself and PPO
synthesized in lab [18], and microcapsule(DMP)-containing
asphalt’s crack face as made and as of 15th day, were taken
X-ray, and Fig. 10 reveals the results. DMP as shown has its specific
peak of 2u at 208 and PPO has it at 158. PPO generally is
noncrystalline but crystalline one also exists [33]. It is considered
that this behavior is related to heat-induced crystallinity [34].
Actually in this case asphalt and microcapsules were mixed at Fig. 8. A fractured microcapsule on the surface of microcapsule(SBS/DMP)-
1608 C. When the diagrams of (c) and (d) are considered, (c) containing asphalt.
 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337 335

Fig. 9. Optical microscope photos of transition of a crack on microcapsule(SBS/DMP)-containing asphalt; (a) as cut, (b) 15 days passed.

resembles (a) due to the fact that (a) is too early stage for DMP to be
PPO. However (d) looks it is a mixture of (a) and (b), that is, a
mixture of PPO and its precursor DMP. This tells that DMP flown
out of the broken microcapsules polymerized very slowly to PPO at
the crack face by aid of oxygen molecules in the air.
Conclusively, a schematic diagram to explain the self-healing
mechanism of these encapsuled asphalts is suggested in Fig. 11.
Microcapsules are mixed with asphalt (a). As time passed, a crack
occurs in the asphalt, microcapsules on the crack propagation path
are also broken and DMP or SBS/DMP solution in the capsule leaks
out, filling the cracked hole (b). In step (b), some of the molecules
flown out of the microcapsules are diffused into the asphalt but
most of them are polymerized to PPO (Fig. 12) in days by the metals
that exist in the cracked area [18] and oxygen molecules in the air.
The polymer, while solidified, adheres to the crack faces,
eventually fills the crack and repairs the damage (c). Adherence
is accompanied by interdiffusion of the molecules from one phase
to the other and randomization of the diffused molecules. Diffusion
and adhesion are much dependent on the intermolecular forces
such as dipole–dipole interaction, van der Waals force and
hydrogen bonding between molecules. Diffusion in (b) and
adhesion in (c) would be promoted by the molecular similarity
between DMP or SBS and asphalt molecules. Therefore if they have
same or similar molecular structure or same or similar polarity,
diffusion and adhesion will be enhanced by strong intermolecular
force. SBS in solid state, which forms an interpenetrating network

Fig. 10. XRD curves of (a) DMP, (b) PPO, (c) microcapsule(DMP)-containing asphalt(as made), (d) microcapsule(DMP)-containing asphalt(15 days after burst).
336 K. Chung et al. / Journal of Industrial and Engineering Chemistry 29 (2015) 330–337

Fig. 11. Schematic diagram showing self-healing process of crack occurred on the surface of microcapsule-containing asphalt; (a) original, (b) as cut, (c) days later.

Fig. 12. Polymerization of poly(phenylene oxide) from 2,6-dimethylphenol.

with PPO can increase the self-healing property due to its nature of
elastic recovery [22]. Fig. 12 shows the polymerization of DMP to
PPO in asphalt. DMP as a polymer-forming monomer is polymer-
ized by metals, such as vanadium, that exist in the asphalt and
catalytic action of oxygen molecules in the air [31]. It is assumed
that the polymerization reaction commences with the creation of a
phenoxy radical by oxidation of DMP, which is coordinated to
metal-amine complex. Two of these radicals coupled by C–O
coupling, followed by tautomerization to create a dimer. The dimer
and larger species can grow by a similar manner adding monomer.
However, the chain extension reaction can also occur by reaction of
two larger species. Therefore, this reaction has components of both
step and chain polymerization chemistry [31].
The healant which has a molecular structure that favors
molecular interaction with asphalt molecules will promote the
healing. In that sense, the reversible ionic bonding, reversible
hydrogen bonding and nanoparticles are thought to be promising
to improve the self-healing ability of asphalt binder and in this way
increase the service life.
Acknowledgement
The authors thank the Korea Agency for Infrastructure Technol-
ogy Advancement (grant no. 12CCTl-C063988-01-000000) for
providing financial support.

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