3

biomimetics
Review
Biomimetic Self-Healing Cementitious Construction
Materials for Smart Buildings
Kwok Wei Shah * and Ghasan Fahim Huseien
Department of Building, School of Design and Environment, National University of Singapore,
Singapore 117566, Singapore; eng.gassan@yahoo.com
* Correspondence: bdgskw@nus.edu.sg; Tel.: +65-9366-6795

Received: 31 July 2020; Accepted: 5 October 2020; Published: 8 October 2020
Abstract: Climate change is anticipated to have a major impact on concrete structures through
increasing rates of deterioration as well the impacts of extreme weather events. The deterioration
can affect directly or indirectly climate change in addition to the variation in the carbon dioxide
concentration, temperature and relative humidity. The deterioration that occurs from the very
beginning of the service not only reduces the lifespan of the concretes but also demands more cement
to maintain the durability. Meanwhile, the repair process of damaged parts is highly labor intensive
and expensive. Thus, the self-healing of such damages is essential for the environmental safety and
energy cost saving. The design and production of the self-healing as well as sustainable concretes are
intensely researched within the construction industries. Based on these factors, this article provides
the materials and methods required for a comprehensive assessment of self-healing concretes.
Past developments, recent trends, environmental impacts, sustainability, merits and demerits of
several methods for the production of self-healing concrete are discussed and analyzed.
Keywords: concrete durability; climate change; sustainability; self-healing technology
1. Introduction
Human settlements are dependent on infrastructure systems (e.g., buildings, transport, energy,
water, communication) to mediate a wide range of human activities. [1]. Globally, infrastructure
made of concrete (e.g., bridges, buildings, wharves, etc.) is susceptible to deterioration due to the
ever-increasing carbon dioxide levels, temperature, and relative humidity [2]. Concrete is primarily
made up of cement, the production of which has major implications for the climate change, especially as
it appears that the demand for cement is relentless. The durability and lifespan of concrete structures
under different weather conditions are influenced greatly by the high sensitivity of the cement materials
to harsh environmental conditions that can cause concrete expansion and eventual cracking [3,4].
In turn, severe structural issues can arise from the concrete cracking. Thus, exceptionally durable
smart concrete based on self-repair technology has been developed in response to the ever-greater
specifications regarding the durability that must be satisfied by these concrete structures [5].
The impact of climate change on human life and ecosystems can be varied and manifest either in
a direct or indirect manner. These include the increasing sea levels, intensification in the rate and/or
severity of extreme weather phenomena, increase in the frequency of heat waves, and enhanced
rate of precipitation. Thus, from the perspective of engineering, more and more research attention
must be directed towards the effect of climate change on the structural features of the concretes.
Simultaneously, risk-based techniques can effectively be employed to evaluate how the viable strategies
of climate adaptation produce an economic benefit. For example, a model for improving the hurricane
risk evaluation was developed by Bjarnadottir et al. [6] by taking into account the effect of climate
change on the intensity and/or frequency of hurricanes. Meanwhile, the stochastic method suggested
Biomimetics 2020, 5, 47; doi:10.3390/biomimetics5040047 www.mdpi.com/journal/biomimetics

Biomimetics 2020, 5, 47 2 of 22
by Bastidas-Arteaga et al. [7] for the concrete structures was intended to facilitate the investigation of
the impact of global warming on chloride ingress, although the study was limited to the incipient phase
of corrosion. In a different study, Stewart and Peng [8] undertook a preliminary risk and cost–benefit
assessment related to the adaptation measures intended to counteract the impact of the carbonation of
reinforced concrete structures (RCs). The effect of climate change on the concrete structure’s durability
in various regions has also been explored in many recent studies. For instance, the contribution of
climate change to the concrete deterioration triggered by corrosion was examined by Stewart et al. [9]
and Wang et al. [10]. They considered a probabilistic method for evaluating corrosion-related cracking
and spalling related to the effect of climate change on regions with distinct geographical conditions.
Additionally, the impact of climate change on carbonation in Toronto and Vancouver (Canada) was
the focus of the study by Talukdar et al. [11], wherein the carbonation depths were found to increase
by around 45% over a period of a century. On the downside, the study disregarded the ambiguities
associated with climate, materials, and models and failed to estimate the extent to which the concrete
infrastructure deterioration and safety were influenced by the carbonation.
The durability of a material is typically aided by the self-repair capability, especially
in challenging situations for human intervention, like constructions situated in areas with
deleterious physical and chemical conditions [12–14]. Another use of self-repair is the protection of
material properties, particularly in kinetic and thermodynamic conditions supporting large defect
densities, like nanostructures. Nanomaterials always have superior functional characteristics, and,
unlike traditional materials, they display a quicker rate of deterioration because of the high content of
interfacial atoms. A wide range of nanosystems can be created through the integration of numerous
functional nanostructures with some constituents added to provide the self-repairing capability.
Indeed, by comparison to the development of a nanosystem with greater robustness, such an approach
is quite basic [15]. The fast innovations in nanoscience and nanotechnology have recently revolutionized
the development of materials with self-repair capability, including nanomaterials, which consist of
particles of less than 500 nm in size. In such materials, degeneration recovery occurs without external
intervention. However, external stimuli (e.g., temperature) can activate self-repair as well, which is the
case with systems known as non-autonomic self-healing materials [16].
The purpose of the present study is to review the current investigations on concrete structures
based on various nanomaterials with self-repair capabilities and their implications for future uses in
sustainable projects. In short, this presentation consists of three parts. First, it is argued that unlike
standard concretes, self-repairing concretes are more eco-friendly and can reduce pollution levels,
thereby enabling the construction industry to move towards a greater sustainability and intelligent
development. The second part deals with several effective and detailed self-repair methods with
comparative analysis of the advantages and disadvantages of each method. The last part involves the
self-repairing systems that are proposed as viable options of concrete self-recovery mechanisms in
response to corrosion, damage, and cracking.
2. Concrete Performance in Aggressive Environments

Economically, the serviceability of building materials is of great importance, especially in
contemporary infrastructures and constituent parts. In the context of urban development, the most
commonly employed concrete materials have to comply with the requirements of the standard codes
of practice with regard to strength and durability [17–20]. For instance, the serviceability of the
concrete material in use can be reduced by factors such as suboptimal planning, low capacity or
overload, flaws in the material design and structures, incorrect building practices or substandard
maintenance as well as the lack of knowledge about engineering [21,22]. The concrete structures
used in construction industries require an extra improvement because they deteriorate rapidly
during the lifespan. This deterioration is due to a range of both extrinsic and intrinsic processes
related to the chemical, physical, thermal, and biological nature [2,23]. Furthermore, the impact
of inadequate use and environmental conditions on how concrete performs has been highlighted
harsh chemicals (e.g., chloride) to penetrate and reach the steel reinforcement bar. After reacting with
water and oxygen these chemicals produce corrosion [28]. Figure 1 illustrates a basic representation
of the occurrence of corrosion in reinforced concrete.
Cracks are detrimental not only in terms of facilitating corrosion, but also concerning the
aesthetics because they make the porous structure in the concrete visible, expanding in size if no
remedial action is taken. The hazardous chemicals can permeate concrete through the large cracks,
leading to the chemical or physical deterioration of the concrete. However, it is not possible to
completely prevent
in many studies micro-cracks
[24–27]. Within in the concreteindustries,
construction because itthe
is too expensiveofinthe
prevention terms
steelofreinforcement
maintenance
and repairs [28]. Consequently, an additional funding allocation is needed for
exposure to hazardous chemicals such as corrosive agents depends significantly on the concrete.maintenance work
with regardthe
In general, to the
steelnecessary materials
reinforcement and skilled
becomes exposedworkers. Basedason
to corrosion these factors,
a result of crackitformation
is realizedinthat
the
materials with self-repair capability can make a substantial difference by repairing
concrete, enabling harsh chemicals (e.g., chloride) to penetrate and reach the steel reinforcement the cracks
bar.
automatically
After reacting and withthus notand
water only reducethese
oxygen the expenditure, but also
chemicals produce increase [28].
corrosion the lifespan
Figure 1ofillustrates
concrete
structures.
a basic representation of the occurrence of corrosion in reinforced concrete.
Figure
Figure 1.
1. Process
Process of
of aggressive
aggressive solution
solution penetration.
penetration.
Cracks
3. Crack are detrimental
Problems in Concrete not only in terms of facilitating corrosion, but also concerning the aesthetics
because they make the porous structure in the concrete visible, expanding in size if no remedial action
The formation of cracks in concrete is a major issue that must be addressed adequately. The
is taken. The hazardous chemicals can permeate concrete through the large cracks, leading to the
drying-related shrinkage, thermal contraction, external or internal restraint to shortening, subgrade
chemical or physical deterioration of the concrete. However, it is not possible to completely prevent
settlement, and overloading can all determine the formation of cracks. Although a complete
micro-cracks in the concrete because it is too expensive in terms of maintenance and repairs [28].
avoidance of crack formation is nearly impossible, some methods are available for mitigating such
Consequently, an additional funding allocation is needed for maintenance work with regard to the
issues. The main points at which cracks form are prior to and following the concrete hardening [29].
necessary materials and skilled workers. Based on these factors, it is realized that materials with
In order to prevent the future degradation that can reduce the use life of concrete structures,
self-repair capability can make a substantial difference by repairing the cracks automatically and thus
knowledge must be acquired about the causes and remedial measures to be adopted in relation to
not only reduce the expenditure, but also increase the lifespan of concrete structures.
crack formation at those crucial moments.
The settlement
3. Crack Problems in ofConcrete
concretes is the key determinant of the formation of pre-hardening cracks. It
starts when the water is lost in the plastic state. Factors including the lack of adequate vibration, high
slumpsThe formation
associated withof exceedingly
cracks in concrete is a major
wet concretes issue that
or insufficient must of
covering bethe
addressed
embeddedadequately.
items (for
The drying-related shrinkage, thermal contraction, external or internal restraint
example steel reinforcement) or at the margin of the concrete are responsible for the settlement to shortening, subgrade
settlement, and overloading can all determine the formation of cracks. Although
cracking. In addition, plastic shrinking can engender the pre-hardening cracking as well [30]. Such a complete avoidance
of crack
cracks formation
usually occuris in
nearly impossible,
the slabs prior tosome methods
the final are available
finishing and under for various
mitigating such issues.
environmental
The main points
conditions at which
including strong cracks
wind,form
loware prior to and
humidity, and following
high daytime the concrete hardening
temperatures. These[29]. In order
conditions
to prevent the future degradation that can reduce the use life of concrete structures,
promote the rapid evaporation of moisture from the surface and thus determine a greater surface knowledge must
be acquired about the causes and remedial measures to be adopted in relation
shrinkage compared to the interior of the concrete [31]. The surface shrinkage is restrained by the to crack formation at
those crucial
interior moments.
concrete, leading to the occurrence of stresses higher than the tensile strength of the concrete
which, in turn, leadsoftoconcretes
The settlement the formationis theofkey determinant
cracks of the The
at the surface. formation
lengthof ofpre-hardening
the cracks relatedcracks.
to
It starts when the water is lost in the plastic state. Factors including the lack of
plastic shrinkage is variable, but they frequently reach the mid-depth of the slab. Such cracks can be adequate vibration,
high slumps
attenuated associated
through withwhich
fogging, exceedingly wet implemented
is generally concretes or insufficient covering
at the construction of the embedded
site.
itemsThe(forfactors
example steel reinforcement) or at the margin of the concrete are
that can stimulate crack formation and post-hardening of concrete include drying- responsible for the
settlement
related cracking.thermal
shrinkage, In addition, plastic shrinking
contraction, and subgradecan engender
settlement. theThe
pre-hardening
strategy ofcracking
insertingasregularly
well [30].
Such cracks usually occur in the slabs prior to the final finishing and under
spaced construction joints is usually applied to avoid shrinkage and manage the crack location. Forvarious environmental
conditions including strong wind, low humidity, and high daytime temperatures. These conditions
promote the rapid evaporation of moisture from the surface and thus determine a greater surface
shrinkage compared to the interior of the concrete [31]. The surface shrinkage is restrained by the
interior concrete, leading to the occurrence of stresses higher than the tensile strength of the concrete
which, in turn, leads to the formation of cracks at the surface. The length of the cracks related to
plastic shrinkage is variable, but they frequently reach the mid-depth of the slab. Such cracks can be
attenuated through fogging, which is generally implemented at the construction site.
The factors that can stimulate crack formation and post-hardening of concrete include
drying-related shrinkage, thermal contraction, and subgrade settlement. The strategy of inserting
Biomimetics 2020, 5, x FOR PEER REVIEW 4 of 21

regularly spaced construction joints is usually applied to avoid shrinkage and manage the crack
location. For instance, the joints can be inserted in such a way as to determine the formation of the
instance, the joints can be inserted in such a way as to determine the formation of the cracks in
cracks in locations where they can be anticipated without difficulty. Furthermore, the number of cracks
locations where they can be anticipated without difficulty. Furthermore, the number of cracks can be
can be minimized through the introduction of horizontal steel reinforcement that can further hinder
minimized through the introduction of horizontal steel reinforcement that can further hinder
excessive crack expansion.
excessive crack expansion.
4. Sustainability of Self-Healing Concrete
4. Sustainability of Self-Healing Concrete
Self-repair technology is a new innovation in the concrete industry that refers to materials having
Self-repair technology is a new innovation in the concrete industry that refers to materials
high quality and the ability to repair damage on their own without any external interference. In fact,
having high quality and the ability to repair damage on their own without any external interference.
this technology is introduced in order to satisfy the demands for reduction in expenditure related to
In fact, this technology is introduced in order to satisfy the demands for reduction in expenditure
concrete structure repair and maintenance [15]. Intense interest has been generated by this technology
related to concrete structure repair and maintenance [15]. Intense interest has been generated by this
in the last ten years due to its potential use in building structures. Self-repair technology is also
technology in the last ten years due to its potential use in building structures. Self-repair technology
known as autonomic healing, autonomic repair and self-healing [32,33]. The main applications of this
is also known as autonomic healing, autonomic repair and self-healing [32,33]. The main applications
technology at the moment are the repair of cracks to restore mechanical strength and automatic crack
of this technology at the moment are the repair of cracks to restore mechanical strength and automatic
repair to avoid extra financial expenditure and necessity of more raw materials [34].
crack repair to avoid extra financial expenditure and necessity of more raw materials [34].
To make the concrete structures more serviceable and expand their use life, crack repair is
To make the concrete structures more serviceable and expand their use life, crack repair is
essential. A material with self-repair capabilities is referred to as an intelligent or smart material,
essential. A material with self-repair capabilities is referred to as an intelligent or smart material,
meaning that it systematically integrates both the construct of information and physical indexes like
meaning that it systematically integrates both the construct of information and physical indexes like
strength and durability [35], affording material functionality at a higher level. Thus, a smart material
strength and durability [35], affording material functionality at a higher level. Thus, a smart material
is able to regulate itself, having a capacity for detection and response as well as controlled delivery
is able to regulate itself, having a capacity for detection and response as well as controlled delivery
of the response. The innate ability of the natural materials and their mechanical properties to adapt
of the response. The innate ability of the natural materials and their mechanical properties to adapt
intelligently has been explored in earlier studies [36]. Conversely, human-made smart materials are
intelligently has been explored in earlier studies [36]. Conversely, human-made smart materials are
yet to fully mature and their applications are only restricted to medicine, bionics, and aeronautics
yet to fully mature and their applications are only restricted to medicine, bionics, and aeronautics or
or astronautics.
astronautics.
Figure 2 shows a schematic diagram of the main mechanisms of self-healing concrete.
Figure 2 shows a schematic diagram of the main mechanisms of self-healing concrete. The
The formation of calcium carbonate from calcium hydroxide, settlement of debris and loose cement
formation of calcium carbonate from calcium hydroxide, settlement of debris and loose cement
particles in presence of water, hydration of un-hydrated cementitious particles, and further swelling of
particles in presence of water, hydration of un-hydrated cementitious particles, and further swelling
the hydrated cementitious matrix are depicted [37]. It is shown that a different self-healing reaction
of the hydrated cementitious matrix are depicted [37]. It is shown that a different self-healing reaction
can occur depending on the self-healing agent used in the concrete. For instance, the use of bacteria as
can occur depending on the self-healing agent used in the concrete. For instance, the use of bacteria
the self-healing agent can lead to the generation of calcium carbonate because of the chemical reactions
as the self-healing agent can lead to the generation of calcium carbonate because of the chemical
between bacteria, oxygen, and water. The bacteria produce a calcite participate via these reactions.
reactions between bacteria, oxygen, and water. The bacteria produce a calcite participate via these
Other expansive self-healing agents can fill up the cracks via swelling of the materials, thus repairing
reactions. Other expansive self-healing agents can fill up the cracks via swelling of the materials, thus
the concrete automatically.
repairing the concrete automatically.
Figure2.2. Main
Figure Main mechanisms
mechanisms of
of autogenous
autogenous healing
healing[37].
[37].
Onetype
One typeofofenergy
energy technology
technology considered
considered withwith great
great potential
potential in making
in making building
building structures
structures more
more sustainable
sustainable and efficient
and energy energy is
efficient
the lowiscarbon
the low carbon
emission andemission and energy-efficient
energy-efficient building
building material with
material with self-repair capabilities. Sustainable development is geared towards the
self-repair capabilities. Sustainable development is geared towards the careful management of human careful
management of human activities to ensure the future survival of humanity on this planet whilst
avoiding any disruption to the ecological equilibrium [38]. Therefore, economic security,
environmental safety, and societal benefits are the pillars of sustainability that have to be upheld for
safeguarding biodiversity and balancing ecosystems. Within the current industry-dominated world,
activities to ensure the future survival of humanity on this planet whilst avoiding any disruption
to the ecological
Biomimetics 2020, 5, x equilibrium
FOR PEER REVIEW [38]. Therefore, economic security, environmental safety, and societal 5 of 21
benefits are the pillars of sustainability that have to be upheld for safeguarding biodiversity5 and
Biomimetics 2020, 5, x FOR PEER REVIEW of 21
balancing
dedicated ecosystems.
efforts are being Within madethe current
in numerousindustry-dominated world, dedicated
fields (e.g., engineering, science,efforts are being
policy-making,
dedicated
made in efforts
numerous are being
fields made
(e.g., in numerous
engineering, fields
science, (e.g., engineering,
policy-making,
architecture) to achieve the resourceful implementation of sustainability to attenuate the adverse science,
architecture) policy-making,
to achieve the
architecture)
resourceful
effects of human to achieve
implementation the resourceful
activities onofecosystems.
sustainability implementation
to attenuate
Regarding of sustainability
the adverse
construction to attenuate
effects sustainability
materials, the
of human activities adverse
impliesona
effects
low of human
ecosystems.
environmental activities
Regarding impact onthe
of ecosystems.
construction materials Regarding
materials, construction
sustainability
[39,40]. In this implies
context, materials, sustainability
a low attention
growing environmental is being implies
impact toa
paid of
lowmaterials
the environmental
self-repair [39,40].impact
technology this of
Inbecause the
context, materials
it can growing
diminish [39,40]. In this
attention
material context,
paidgrowing
isdeterioration,
being to expand attention
self-repair life,isand
usetechnologybeing paid to
because
eliminate
self-repair
it can diminish
maintenance technology because
material deterioration,
expenditure it can
[41,42]. Hence, diminish
expand material
use life,
self-repair deterioration,
and eliminate
technology expand
maintenance
can make use life, and
expenditure
construction eliminate
materials [41,42].
and
maintenance
Hence, expenditure
self-repair technology [41,42].
can Hence,
make self-repair
construction technology
materials can
and
concrete more sustainable by lengthening its use life and decreasing the ordinary Portland cement make construction
concrete more materials
sustainable and
by
concrete
lengthening
(OPC) demand more sustainable
its use
andlife by lengthening
and decreasing
consumption, its
the ordinary
improving use
energylife and
Portland
efficiencydecreasing
cementand (OPC)the
lowering ordinary
demand Portland
and consumption,
pollution levels. cement
(OPC) demand
improving energy and consumption,
efficiency improving
and lowering energylevels.
pollution efficiency and lowering pollution levels.
5. Mechanism of Self-Healing in Cementitious Materials
5. Mechanism
5. Mechanism of of Self-Healing
Self-Healing in in Cementitious
CementitiousMaterialsMaterials
In the human body, skin and tissues are capable of repairing themselves through replacements
Inthe
In
of damagedthehuman
human
areas basedbody,skin
body, skin
on andtissues
and
nutrient tissues are
uptake.are capable
capable
Similarly,ofof repairing
repairing
the themselves
themselves
essential products through
through
that replacements
replacements
serve as nutrients of
of damaged
damaged areas
areas based based
on on nutrient
nutrient uptake.uptake. Similarly,
Similarly, the the essential
essential products
products
in the cement-based materials with self-repair capability may enable these materials to repair the that that
serve serve
as as
nutrients nutrients
in the
in the cement-based
cement-based
damage materials
or deterioration materials
with
(Figure with
self-repair self-repair
3). Amplecapability capability
researchmay enable
has may
been enable
these these
materials
conducted materials
to
in recentrepair
timesthetotorepair
damage the
discoveror
damage or
deterioration deterioration
(Figure 3). (Figure
Ample 3).
researchAmplehas research
been has
conducted beenin conducted
recent
new methods for achieving an effective self-repair material alongside the durability of the cement- times intorecent
discovertimesnew to discover
methods
new
for
based methods
achieving
materials. anforeffective
achieving
Figure an effective
self-repair
4 illustrates self-repair
material
an overview alongsidematerial
of such the alongsideofthe
durability
methods. thedurability
cement-based of the cement-
materials.
based materials. Figure 4 illustrates
Figure 4 illustrates an overview of such methods. an overview of such methods.
Figure 3. Healing of microcracks in concrete cover due to continuing hydration of unhydrated cement
Figure 3. Healing
3.
Figure[43].
nuclei Healing of
of microcracks
microcracks in
in concrete
concretecover
cover due
due to
to continuing
continuing hydration
hydrationof
of unhydrated
unhydratedcement
cement
nuclei [43].
nuclei [43].
Figure
Figure 4. Developed strategies
4. Developed strategies for
for self-healing
self-healing in
in cement
cement based
based materials.
materials.
Figure 4. Developed strategies for self-healing in cement based materials.
5.1. Expansive Agents and Mineral Admixtures
5.1. Expansive Agents and Mineral Admixtures
5.1. Expansive
In a studyAgents
by KishiandetMineral
al. [44],Admixtures
it was found that cementitious materials like Al2 O3 –Fe2 O3 -tri (Aft),
In a study by Kishi et al. [44], it was found that cementitious materials like Al2O3–Fe2O3-tri (Aft),
Al2 O3In
–Fe O
2 3 -mono (Afm), and calcium carbonate (CaCO3 ) werematerials
created like
in cracked concrete and
Al2O3–Fea2study
O3-monoby Kishi
(Afm), et al.
and [44], it was carbonate
calcium found that(CaCO
cementitious Al2O3–Fe 2O3-tri (Aft),
3) were created in cracked concrete and
Ca(OH)
Al2O3–Fe 2 2crystal
O3-monoair (Afm),
voids. Theand working
calcium assumption argued
carbonate (CaCO for the leaching out of such hydration
3) were created in cracked concrete and
Ca(OH) 2 crystal air voids. The working assumption argued for the leaching out of such hydration
Ca(OH)
yields and2 crystal air voids. The working assumption argued for the leaching out of such hydration
renewed crystallization in flow water via fractures. In line with this, a range of repair
yields and renewed
agents, including crystallization
expansive in flow water and
agents, geo-materials, via fractures. In line with
chemical mixtures this, with
together a range
theirofblends
repair
agents,
were including
used expansive
to assess agents, geo-materials,
the performance and
of concrete in chemical
terms of itsmixtures together
ability to repair with
itself their blends
[44–46]. In
were used to assess the performance of concrete in terms of its ability to
addition, comparative analysis was undertaken between the reference specimen and the specimen repair itself [44–46]. In
addition, comparative analysis was undertaken between the reference specimen and the specimen
yields and renewed crystallization in flow water via fractures. In line with this, a range of repair agents,
including expansive agents, geo-materials, and chemical mixtures together with their blends were
used to assess the performance of concrete in terms of its ability to repair itself [44–46]. In addition,
comparative
with 10% cement analysis was undertaken
content replaced with between
expansive the reference
materials specimen
consistingand of Cthe specimen with 10%
4A3S, CaSO4, and CaO.
cement content replaced with expansive materials
Results showed that the presence of expansive agents in the concreteconsisting of C A
4 3 S, CaSO
beams , and CaO. Resultsthe
4 nearly enabled showed
repair
that the presence of expansive agents in the concrete beams nearly
of an early 0.22 mm crack after more than 30 days with the detection of rehydration yield between enabled the repair of an early
0.22 mm crack after more than 30 days with the detection of rehydration
the cracks. In contrast, for the standard concrete structures, partial repair of the cracks occurred yield between the cracks.
In contrast,
during for the standard
an identical intervalconcrete structures,
of time. Hence, partial repair
in comparison toofthethe cracks occurred
standard concrete,during
a higheranefficiency
identical
interval of time. Hence, in comparison to the standard concrete, a higher
was demonstrated by the expansive agent re-crystallization in the air voids for self-repair [44]. efficiency was demonstrated
by the expansive
Qureshi agent
et al. [26] re-crystallization
provided evidence thatin theconcrete
air voidsmixtures
for self-repair [44]. Qureshi
containing expansive et al.minerals
[26] provided
had a
evidence that concrete mixtures containing expansive minerals had a greater
greater capability of repairing themselves. Representing a marker of the state of the cement mixture capability of repairing
themselves.
at a given age, Representing
the hydrationa marker of theenabled
degree state of quantitative
the cement mixtureestimationat a given
of theage, the hydration
cement mixture’s
degree enabled quantitative
performance in terms of self-repair. estimation of the cement mixture’s performance in terms of self-repair.
ItItwas
wasdemonstrated
demonstratedthat thatthethe
geo-polymer
geo-polymer waswasformed
formedduedueto theto addition
the additionof theofgeo-material
the geo-materialwith
awith
content of 71.3% SiO
a content of 71.3% 2 and 15.4% Al O
SiO2 and2 15.4%3 to the expansive material through a separate
Al2O3 to the expansive material through a separate polymerization
of the aluminateof
polymerization and thesilicate
aluminate complexes [45]. complexes
and silicate The presence ofThe
[45]. alkali metals of
presence caused
alkalithe dissolution
metals caused theof
the polymerized aluminate and silicate complexes at the alkaline pH.
dissolution of the polymerized aluminate and silicate complexes at the alkaline pH. As uncovered byAs uncovered by an extensive
examination, the geo-polymer
an extensive examination, gel particles gel
the geo-polymer wereparticles
less than were2 µmlessinthansize2 and
µm ainlarge number
size and of
a large
hydro-garnet or Aft phases
number of hydro-garnet orwere produced
Aft phases were byproduced
cracked interfacial
by cracked phases associated
interfacial phases with the original
associated with
ruptured zone (Figure 5). In comparison to the hydro-garnet
the original ruptured zone (Figure 5). In comparison to the hydro-garnet phase, the dense phase, the dense phase contained
phase
most of themost
contained altered
of thegeo-polymer gel as revealed
altered geo-polymer by the Energy
gel as revealed by the Dispersive
Energy DispersiveX-Ray Analyzer (EDX)
X-Ray Analyzer
spectra. According to additional analysis of the chemical additives,
(EDX) spectra. According to additional analysis of the chemical additives, an improvement was an improvement was achieved
by supplementing
achieved regular concrete
by supplementing regularenclosing
concrete theenclosing
NaHCO3 the , Na2NaHCO
CO3 , and Li22CO
3, Na CO33., Such
and Li composition
2CO3. Such
triggered
composition the triggered
cementitious re-crystallization
the cementitious and concrete and
re-crystallization particle precipitation
concrete [45]. The conclusion
particle precipitation [45]. The
reached was that crack self-repair could be greatly enhanced through the
conclusion reached was that crack self-repair could be greatly enhanced through the addition of addition of sufficient quantities
of carbonates
sufficient and expansive
quantities agents.and expansive agents.
of carbonates
Figure5.
Figure 5. Microstructure
Microstructureof
ofresults
resultsbetween
betweenself-healing
self-healingarea
areaand
andoriginal
originalarea
area[45].
[45].
5.2.
5.2. Hollow
Hollow Fibers
Fibers
Self-repair
Self-repair is made possible
is made possibleby bythe
thehollow
hollowfibers
fibers
as as illustrated
illustrated in Figure
in Figure 6. These
6. These fibersfibers use
use voids
voids constituting a composite network matrix for the storage of certain functional
constituting a composite network matrix for the storage of certain functional constituents of the constituents
of the materials
materials servingserving as agents
as repair repair agents
[47,48].[47,48]. When extrinsic
When extrinsic stresses stresses orcause
or stimuli stimuli cause concrete
concrete structure
structure
deterioration and crack formation, the functional constituents are released from the voids in voids
deterioration and crack formation, the functional constituents are released from the which
in which
they they are
are stored to stored to automatically
automatically heal damage.healThus,
damage.
theseThus, these
hollow hollow
fibers work fibers
akin towork akinintoa
arteries
arteries in a living making
living organism, organism, it making
possible itfor
possible for the materials
the materials in whichintheywhicharethey are embedded
embedded to
to repair
repair themselves [48,49]. For example, the self-repair of polymeric composites
themselves [48,49]. For example, the self-repair of polymeric composites is facilitated by bulk is facilitated by
bulk polymers
polymers [50–53].
[50–53]. The technique
The technique of damage
of damage visual enhancement
visual enhancement was by
was devised devised by Pang
Pang and Bondand
[53]
for the rapid and straightforward detection of the internal damage in the composite structures.
Evidence has been provided that the progress of the healing process can be monitored via the fibers
containing engineering healing materials and labelled with the fluorescent dye.
The technology of crack repair in cementitious materials is based on the same mechanism as the
self-healing biological functions similar to blood coagulation [54,55]. It involves the incorporation of
the functional constituents in delicate fibrous vessels permeating the structural network of the
concrete. The occurrence of deterioration triggers the rupture of the fibers and release of the
Biomimetics
functional 5, 47 materials that activate self-healing. Empirical work has succeeded in making
2020,repair 7 of 22
concrete less porous by incorporating liquid methyl methacrylate (MMA), methacrylic acid methyl
ester[53]
Bond andfor reactive resin
the rapid andinto the hollow polypropylene
straightforward detection of the fibers thatdamage
internal were subsequently
in the composite inserted into the
structures.
concrete [55]. Other researchers investigated the discharge of crack-bridging
Evidence has been provided that the progress of the healing process can be monitored via the fibers cementitious glue from
hollow glass
containing pipettes within
engineering healingthe concrete
materials andinstantly
labelledafter
withthe theflexural test.dye.
fluorescent Compared to the concrete
structures without such glue constituents, those with the
The technology of crack repair in cementitious materials is based on the same glue were capable to mechanism
carry 20% heavieras the
loads.
self-healing biological functions similar to blood coagulation [54,55]. It involves the incorporation
of the The buoyantconstituents
functional process associated withfibrous
in delicate self-repair has permeating
vessels been discussed thein various studies
structural network [54,56,57].
of the
This process was elucidated by inserting hollow fibers in the cementitious
concrete. The occurrence of deterioration triggers the rupture of the fibers and release of the functional network matrix with one
end linked
repair materials to the
that self-repair mediator and
activate self-healing. the other
Empirical work endhastied up. Theinconcrete
succeeded making mixtures
concrete less were
produced
porous and insertedliquid
by incorporating into glass
methyl tubes with 2 mm
methacrylate external
(MMA), diameter acid
methacrylic and methyl
0.8 mmester internal diameter
and reactive
[56]. The self-repair constituent included diluted (27%) and non-diluted
resin into the hollow polypropylene fibers that were subsequently inserted into the concrete [55]. alkali-silicate mixtures and
two components
Other integrating epoxy
researchers investigated resin ofoflow
the discharge viscosity. Next,
crack-bridging loading was
cementitious glueperformed
from hollow until
glassthe
crack mouth opening displacement (CMOD) reached 0.03–2 mm following
pipettes within the concrete instantly after the flexural test. Compared to the concrete structures the load removal. To
determine whether the self-repair capability was enhanced, the cracked
without such glue constituents, those with the glue were capable to carry 20% heavier loads. specimens were subjected to
renewed curing.process
The buoyant A strength recovery
associated withmean ratio of
self-repair has1.1been
anddiscussed
1.5 was respectively
in various studies displayed by the
[54,56,57].
specimens with the repair constituent of dilute and non-dilute alkaline
This process was elucidated by inserting hollow fibers in the cementitious network matrix with silica solution, unlike the
specimens without repair constituent. In contrast, the strength recovery
one end linked to the self-repair mediator and the other end tied up. The concrete mixtures were ratio did not show significant
gains forand
produced theinserted
specimensinto with
glass epoxy resin.
tubes with In fact,
2 mm it was
external aroundand
diameter three times
0.8 mm lower diameter
internal than the [56].ratio
associated with direct mixing and manual injection of resin into areas
The self-repair constituent included diluted (27%) and non-diluted alkali-silicate mixtures and twowith cracks. It was argued that
the two components
components integratinghad not resin
epoxy been of properly blendedNext,
low viscosity. and loading
stirred, that
was caused
performed the until
resin the
to harden
crack
inadequately and resulting in a low repair ratio. Another possible
mouth opening displacement (CMOD) reached 0.03–2 mm following the load removal. To determine explanation was that the pipes still
contained
whether thethe residualcapability
self-repair epoxy as one wasend was blocked.
enhanced, the cracked specimens were subjected to renewed
curing.According
A strengthtorecovery
Joseph [57],
meanapart ratio from
of 1.1 aandfew 1.5negligible differences
was respectively the testing
displayed by theprotocol
specimens was
identical. The conduit of repair mediator (ethyl cyanoacrylate) was represented
with the repair constituent of dilute and non-dilute alkaline silica solution, unlike the specimens by bent plastic tubes
with 4 repair
without mm external diameter
constituent. and 3 mm
In contrast, internal recovery
the strength diameter.ratio Thedidconclusion
not showreachedsignificantwasgains
that forself-
repair
the can effectively
specimens with epoxybe accomplished
resin. In fact,basedit wason the external
around provision
three times lowerofthan
suchthe a repair constituent.
ratio associated
with direct mixing and manual injection of resin into areas with cracks. It was argued that following
A considerable improvement was noted in the post-crack stiffness, peak load, and ductility the two
the damage repair. As suggested by the observations made during and
components had not been properly blended and stirred, that caused the resin to harden inadequately after assessment, the capillary
and resulting in a low repair ratio. Another possible explanation was that the pipes still contained theof
suction and gravitational effects made ethyl cyanoacrylate a suitable adhesive agent capable
permeating
residual epoxy anasextensive
one end was area blocked.
of the surfaces with cracks.
Figure6.6.Schematic
Figure Schematicrepresentation
representationofofself-healing
self-healingprocesses
processesusing
usinghollow
hollowfibers [58].
fibers [58].
According to Joseph [57], apart from a few negligible differences the testing protocol was identical.
The conduit of repair mediator (ethyl cyanoacrylate) was represented by bent plastic tubes with
4 mm external diameter and 3 mm internal diameter. The conclusion reached was that self-repair can
effectively be accomplished based on the external provision of such a repair constituent. A considerable
improvement was noted in the post-crack stiffness, peak load, and ductility following the damage
repair. As suggested by the observations made during and after assessment, the capillary suction
and gravitational effects made ethyl cyanoacrylate a suitable adhesive agent capable of permeating
an extensive area of the surfaces with cracks.
5.3. Bacteria as Self-Healing Agent

Biological mechanisms for repair involving the introduction of bacteria into the concrete have
been recently suggested [59–63]. During the middle of the 1990s, a sustainable method for healing
cracks in concrete was proposed by Gollapudi [64] that involved the introduction of ureolytic bacteria
to speed up CaCO3 precipitation in the concrete micro-crack zones. Several parameters were employed
to describe this process, including the amount of dissolved inorganic carbon, the pH of the material,
the levels of calcium ions, and nucleation site accessibility. The walls of the bacterial cells represented
the nucleation sites, while the other parameters were regulated by the bacterial metabolism [60].
Tittelboom and coworkers [60] used bacteria in the concrete to generate an enzyme called urease that
could catalyze urea (CO(NH2 )2 ) into the ammonium ions (NH4 + ) and carbonate radicals (CO3 −2 ).
In the chemical reactions 1 mol of urea underwent intracellular hydrolyses to 1 mol of carbonate and
1 mol of ammonia following Path I. Then, carbamate was hydrolyzed spontaneously to form one extra
mole of ammonia and carbonic acid via path II. These products later formed 1 mol of bi-carbonate
(HCO3 − ) and 2 moles of ammonium (NH4 + ) and hydroxide (OH−1 ) ions (Path III and IV). Path IV
and V was responsible for the enhancement of pH, drifting the bicarbonate equilibrium to form
carbonate ions.
CO(NH2 )2 + H2 O → NH2 COOH+NH3 Path I
NH2 COOH + H2 O → NH3 + H2 CO3 Path II
H2 CO3 + H2 O → HCO3 − + H+1 Path III
2NH3 + 2H2 O → 2NH4 + + 2OH−1 Path IV
HCO3 − + H+1 + 2NH4 + + 2OH−1 → CO3 −2 + 2NH4 + + 2H2 O Path V
The walls of the bacterial cells had a negative charge, so cations from the surrounding environment
can be accepted by the bacteria, with the deposition of Ca+2 on the cell wall surface. The reaction
between Ca2+ and CO3 −2 resulted in the precipitation of CaCO3 on the surface of the cell wall (Path VI
and VII), thus providing active nucleation sites. The repair of surface cracks was made possible through
this method of bacterial-based localized CaCO3 precipitation as illustrated in Figure 7.
Ca+2 + Cell → Cell-Ca+2 Path VI
Cell-Ca+2 + CO3 −2 → Cell-CaCO3 Path VII

reaction between Ca2+ and CO3−2 resulted in the precipitation of CaCO3 on the surface of the cell wall
(Path VI and VII), thus providing active nucleation sites. The repair of surface cracks was made
possible through this method of bacterial-based localized CaCO3 precipitation as illustrated in Figure
7.
Ca+2 +2020,
Biomimetics → Cell-Ca+2 Path VI
Cell5, 47 9 of 22
Cell-Ca + CO3−2 → Cell-CaCO3 Path VII
+2
Biomimetics 2020, 5, x FOR

Figure
Figure 7. PEER REVIEW
7. Typical
Typical crack-healing
crack-healing processes
processes via
via immobilized
immobilized bacteria in concretes [59]. 9 of 21
5.4.
5.4. Microencapsulation
Microencapsulation
Inspired
Inspiredby bythethenatural phenomena,
natural phenomena, several encapsulation
several materials
encapsulation have been
materials havemade
beenwith diverse
made with
sizes,
diversefrom macro-
sizes, from to nano-scale.
macro- At the macroscopic
to nano-scale. level, natural
At the macroscopic encapsulation
level, natural in its most
encapsulation in itsbasic
most
form
basic is embodied
form is embodiedby thebybird
the eggs or seeds.
bird eggs Whereas,
or seeds. Whereas,at the micro
at the level
micro natural
level encapsulation
natural encapsulation is
embodied by an egg or seed cell [65–67]. The starting point of the microencapsulation
is embodied by an egg or seed cell [65–67]. The starting point of the microencapsulation development development
was
was the
the creation
creation of dye-containing
dye-containing capsules.
capsules. Numerous
Numerousnovel noveltechnologies
technologieshavehave been
been introduced
introduced in
in different
different fieldsofofapplications
fields applications[68].
[68].Microencapsulation
Microencapsulationisisnot notaa separate
separate component,
component, but can be be
understood
understood as as insertion
insertion ofof solid
solid granules
granules ofof the
the order
order of
of micrometers,
micrometers, liquid
liquid drops
drops oror gases
gases into
into the
the
inert
inert shell,
shell, affording
affording protection
protection against
against the
the activity
activity of
of external
external agents
agents [69,70].
[69,70]. This
This was
was thethe basis
basis of of
microencapsulation with self-repair capability [69,71]. The mechanism of self-repair
microencapsulation with self-repair capability [69,71]. The mechanism of self-repair is illustrated in is illustrated in
Figure
Figure 8a,b.
8a,b. The
The embedded
embedded microcapsules
microcapsules break when when thethe cracks
cracks are
are formed,
formed, causing
causing release
release of
of the
the
repair
repair agent into the the crack
cracksurfaces
surfacesthrough
throughcapillary
capillaryaction,
action, followed
followed bybythethe interaction
interaction between
between the
the repair
repair agent
agent andand incorporated
incorporated catalyst,
catalyst, therebytriggering
thereby triggeringpolymerization
polymerizationand andsealing
sealing ofof cracks.
Figure
Figure 8b8belucidates
elucidatesthe themicrocapsule
microcapsulerupturing
rupturingmechanism.
mechanism.
Figure 8.8. (a) The

Figure The microencapsulation
microencapsulation approach and
and (b)
(b) typical
typical Field
Field Emission
Emission Scanning
Scanning Electron
Electron
Microscope(FESEM)
Microscope (FESEM)micrograph
micrographof
ofaacracked
crackedmicrocapsule
microcapsule[69].
[69].
In a study conducted by Nishiwaki [72], epoxy resin was used as a repair material packed into
the microcapsules with the incorporation of a urea-formaldehyde formalin shell of size 20–70 µm.
The microcapsules were used together with the acrylic resin. The results indicated that self-repair
was successfully achieved by the microcapsules containing sodium silicate [73]. The concrete stacking
In a study conducted by Nishiwaki [72], epoxy resin was used as a repair material packed into
the microcapsules with the incorporation of a urea-formaldehyde formalin shell of size 20–70 µm.
The microcapsules were used together with the acrylic resin. The results indicated that self-repair was
successfully achieved by the microcapsules containing sodium silicate [73]. The concrete stacking
was initially performed nearly to the breaking point prior to removal of the load and subsequent
curing for seven days. In comparison to the reference specimen that exhibited just 10% recovery,
the specimen with 2% sodium silicate microencapsulation regained its strength to a proportion of
up to 26%. It was concluded that the upper strength recovery ratio was possible by increasing
the concentration of the repair material. Meanwhile, Yu et al. [74] prepared single-component
microcapsules with toluene-di-isocyanate (TDI) and paraffin serving as the repair agent and shell,
respectively. The findings revealed that encapsulation of TDI within the paraffin shell was successful
and a better self-repair capability was demonstrated by mortars containing the microcapsules.
5.5. Shape Memory Materials as Self-healer

The integration of functional materials such as shape memory alloys (SMAs) or shape memory
polymers, into cementitious concrete structures to promote self-repair has been advocated in a number
of studies [75–78]. The underlying principle is that crack formation triggers the controlled shrinkage
of these materials, producing a contraction serving to seal the cracks. The shape memory effect was
discovered by Chang and Read and reported that a gold–cadmium (Au-Cd) alloy exhibits a reversible
phase change [78]. Since then, several SMAs with exceptional thermo-mechanical and thermo-electrical
properties have been developed [79]. For example, nitinol is a highly elastic alloy that demonstrates
the shape memory effect and capable of reversing to its pre-established form upon heat exposure [80].
Its super-elasticity permits to withstand a major inelastic deformation and returns to its original form
once the load is removed. Song and Mo [81] produced an intelligent reinforced concrete (IRC) by
employing the SMA wires. More specifically, stranded martensite wires of the SMAs were used
to accomplish post-tension effects in the IRC. The strain distribution in the concrete was obtained
by tracking changes in the electrical resistance of the SMA wires. This allowed detection of the
cracks forming as a result of explosions or earthquakes. The SMA wire electrical heating triggered
contraction thus alleviating the cracks so that the self-repair capability was effective for managing
macro-cracks. The name of the IRC derived from the fact that the concrete structure is sufficiently
smart to recognize self-repair.
Sakai et al. [75] studied the super-elasticity of the SMA wires for concrete beam self-repair and
acknowledged the almost complete recovery of a massive crack. Meanwhile, Jefferson et al. [77]
integrated the shape memory polymers (SMPs) into cementitious materials and showed that early
age shrinkage, thermal effects, and/or mechanical loading can cause the formation of cracks in the
cementitious matrix. The exposure to heat can activate shrinkage of the incorporated SMA tendons,
which in turn generates quantifiable compressive stresses throughout the closed crack surfaces,
thus promoting crack healing. This kind of mechanism of crack closure can make concrete structural
components perform better in terms of self-repair and durability. The deduction derived from
the findings was that crack closure and weak pre-stressing in post-tensioned mortar beams can be
successfully addressed based on incorporation of parallel polymer tendons subjected to shrinking.
Numerous screening tests indicated that the tendons of highest efficiency are the polyethylene
terephthalate (PET) Shrinktite, exhibiting a shrinking potential of around 34 MPa in a controlled
environment with heating up to 90 ◦ C followed by cooling down to ambient temperature. An increase
of about 25% in mortar strength was estimated to be promoted by heating plus additional curing.
5.6. Coating
The supplementary functionalities created by the latest material technology innovations brought
the concept of “intelligent material”, which refers to the ability to effectively respond to extrinsic
stimuli (e.g., temperature, light, humidity). This has led to the successful development and testing
of advanced construction materials such as coatings for concrete with self-repair capabilities and
particular durability qualities [82,83]. For reinforced concrete, such coatings are devised to promote
steel bar self-repair and minimize deterioration due to corrosion. The newest research initiative
of self-repairing coatings has the potential to make a notable contribution to the efforts to combat
contemporary infrastructure degradation. Unlike standard anti-corrosion coatings in which efficiency
is compromised by the slightest coating damage, self-repairing coatings are capable of recovery from
damage. Thus, the efficiency of self-repairing coatings remains unaffected [84]. Therefore, this capability
is likely to extend the use life of steel rebar structures considerably [85]. Chen et al. [86] first explored
the use of self-repairing coatings for steel rebar. Epoxy coatings that were usually applied to the
rebar structures can be substituted with self-repairing coatings, especially in the northeastern regions,
to protect the rebar against the high levels of corrosion.
Identification of the strategies for preventing micro-crack formation in concrete structures
(e.g., roads, bridges, etc.) has been the focus of ample research, but no definitive conclusions have
been reached so far [23,87,88]. The penetration of concrete by water, de-icing salt, and air is facilitated
by cracks. The sub-zero temperatures cause the expansion of frozen water within the cracks, which
thus become larger in size and cause the concrete to deteriorate faster upon exposure to the road salt.
However, self-repairing coatings for the protection of concrete have received far less research attention
than self-repairing coatings with anti-corrosion action for the protection of metal. Several studies
were conducted on self-repairing coatings that trigger self-repair in response to the extrinsic crack
formation or damage. Such coatings frequently incorporate micro containers that break readily in the
presence of disruptive agents. The healing agents within these containers can extend the coating’s
lifespan by sealing the existing cracks. Meanwhile, the containers themselves can take various forms
including polyurethane microcapsules and microfilament tubes, but they rarely impact the coating
mechanical properties. Various promising findings in this field warranted an additional exploration
for the practical uses [33,85,89].
Over the years, diverse organic and inorganic materials have been employed as healing agents to
achieve high performance self-repairing. The protection of rebar against corrosive agents (e.g., water,
salts) commonly relies on epoxy coatings. Studies have also been dedicated to the creation of
polymer coatings capable of activating crack repair in response to external stimuli (e.g., heat,
pH alterations). The heat-responsive coatings became successful and few of them can maintain their
mechanical properties even after repeated heat cycles [90,91]. It has been reported that polyelectrolyte
nanocontainer coatings can respond to changes in the pH within seconds [92]. These types of
coatings have great potential for further applications, especially due to their distinct mechanical
properties that can completely be restored. Particular attention has been directed towards drying
oils like tung oil and linseed oil owing to their excellent repair capabilities and encapsulation [93].
Upon exposure to air, tung oil undergoes polymerization to a coating characterized by toughness,
glossiness, and imperviousness [94–96]. Due to such properties, drying oils are widely incorporated
into paints, varnishes, and printing inks. Samadzadeh et al. [97] accomplished the first encapsulation
of tung oil. Assessment of the microcapsules’ pull-off strength revealed that the urea-formaldehyde
microcapsules adhered to the epoxy matrix more effectively than the industrial standards. In addition,
evaluation of the lifespan by immersing the damaged specimens into sodium chloride solutions yielded
a positive outcome. Compared to epoxy coatings, a nine-fold extension of the use life was achieved by
tung oil microcapsules following the damage.
5.7. Engineered Cementitious Composite

The ultra-ductile fiber-reinforced cementitious composite also called the engineered cementitious
composite (ECC) is a special type of concrete that was introduced at the beginning of the 1990s.
The ECC was continually refined over past two decades [98]. It is highly ductile (3%–7%) and
displays a tight crack size and a relatively reduced amount of fibers that does not exceed 2% by
volume [99]. The distinguishing mechanical quality of the ECC is the metal-like feature. Furthermore,
the ECC can withstand heavy loading following crack formation in the context of auxiliary distortions.
The self-healing notion of the dry related to the bleeding was investigated by Li et al. [100] regarding
the release of chemicals capable of sealing tensile cracks with ulterior air curing. In this manner,
composites without cracks can recover their mechanical properties. However, the self-repair process
was admitted to lack of efficiency in case of the standard concrete, cement or fiber-reinforced concrete
because the tensile crack size is challenging to control in such materials. A decrease in tensile load can
promote the relentless multiplication of local breaks within the crack width, leading to rapid depletion
of the repair agents. Hence, it is necessary to reduce the tensile crack width to within ten of microns
for achieving a successful self-repair. The alternative is to change the mechanical properties of the
composites with the use of glass pipes of extremely large size. This was highlighted by several other
studies that drew attention to the significance of the crack width [101–103].
The notion of self-repair is feasible for the ECC due to the major property of tight crack size control
of this material, as explored by two distinct empirical studies [30]. The first study involved the use of
SEM for in situ testing of the ECC with one empty glass fiber without the healing chemicals under the
condition of the applied load, while the second study involved measurement of the flexural strength of
the ECC incorporated glass fibers with ethyl cyanoacrylate as the sealing agent. To assess the efficiency
of the sealing mediator for repair purposes following the occurrence of deterioration in the load cycles,
both studies were conducted under the materials test system (MTS) load-frames. The SEM images
showed the sensing and actuation processes, while the flexural stiffness recovery was indicative of the
effect of regeneration. It was admitted that prior to implementation, the additional problems must
be addressed.
The self-repair capability of cementitious materials and the use of external chemicals as repair
glue in concrete were investigated by Li et al. [104–106]. They analyzed the concrete matrix and its
interaction with the exposed surroundings. The cracks were induced into the ECC before exposing
it to a range of environmental conditions including water penetration and submersion, wetting and
drying cycles and chloride ions attack. The results revealed almost full recovery of the mechanical and
transport properties, especially for the ECC preloaded with the tensile strain below 1%. Self-repair
was promoted by the minute crack size, low ratio of water to binder, and abundant fly ash (FA) content
via hydration and pozzolanic mechanisms.
Waste matter and/or by-products were employed by Zhou et al. [107] for local production of
ECC materials. Both slag and limestone (LS) powders were used to design a number of mixtures,
which were then subjected to analysis that involved measurement of tensile strain (2–3%) and crack
stiffness. Results indicated that unlike the mixtures studied by Li et al. [105], the mixtures considered
by Zhou et al. [107] had a higher concentration of blast furnace slag (BFS) and LS instead of FA as
well as a higher water-binder ratio (0.45–0.60). It was inferred that a significantly lower amount of
un-hydrated cementitious materials with curing longer than 28 days was used than in the study by
Li et al. [101]. Furthermore, compared to the ECC materials with rich FA content and low ratio of water
to binder, the ECC materials with high BFS and LS content and relatively high water to binder ratio
display similar self-repair capability. This conclusion was derived from the tight crack width, with the
ECC self-repair depending on the availability of un-hydrated cement and additional complementary
products (e.g., BFS). In fact, self-repair was promoted by a low water-cementitious material ratio and
high proportion of cementitious specimen. Moreover, crack size was highlighted as important for
hydration-reliant self-repair as crack sealing could be achieved with minimal use of healing agent and
crack bridging from both sides was facilitated.
Through release of the healing agents, the presence of microencapsulated modules generally
promoted improvement of ECC micro-crack behavior and likelihood of crack formation.
Consequently, the processes of sensing and actuation were made effective via microencapsulation.
As previously mentioned, a considerable importance is attached to the ECC tight crack size as it
minimizes the amount of healing agents needed to seal cracks and makes it easier for these agents to
bridge cracks from both sides. In short, the self-repair capability of the ECC is greater compared to
standard cements because of its higher proportion of cementitious materials and lower ratio of water
to binder.
5.8. Nanomaterials Based Self-Healing Concrete

In the concrete industry, the use of self-repairing materials is still a relatively recent innovation.
These materials refer to the materials that contain cement and are capable of autonomous recovery from
deterioration caused by various factors. Simultaneously, a considerable interest is currently being raised
by the possibility of producing sustainable concrete using nanomaterials. Thus, concrete can be made
more durable and sustainable by integrating self-repair and nanomaterial technologies [108,109]. In the
context of self-repair, nanomaterials have been employed primarily to mitigate steel bar corrosion in
reinforced concrete. For instance, Koleva [108] indicated that the use of nanomaterials with customized
qualities, such as core-shell polymer vesicles or micelles can help reinforced concrete to perform
better. However, the use of nanomaterials in concrete with self-repair capabilities has not been
extensively studied.
Qian et al. [110] investigated curing under air, carbon dioxide, and water in both wet and dry state,
as well as the impact of nanoclay with water employed as hydration-related inner water furnishing
agent on micro-cracks. The results revealed that the addition of nanoclay and more suitable amounts of
cementitious materials into the mixtures could significantly enhance the repair capability. In addition,
every air-cured mixture displayed satisfactory repair as attested by the absence of final crack formation
at the new site. Meanwhile, Hua [63] discovered that the addition of super absorbent polymer capsules
with water as inner pool for supplementary hydration afforded the ECC a greater self-repair capacity.
Furthermore, various repair products were identified over the cracked facades, but there were no
obvious repaired cracks. It was concluded that the self-repair mechanism does not significantly affect
the cracks. Access to sufficient water or moisture was also stressed as being important as it not only
served as the reactant for supplementary hydration, but also facilitated the transport of ions.
6. Self-Healing in Fiber-Reinforced Concrete

The concrete composite is made of binders, fine and coarse aggregates, and short length
discontinuous fibers. These fibers can significantly enhance the impact resistance, ductility, and energy
absorption of concrete in addition to the higher values of splitting tensile and flexural strengths dispersed
in the concrete mixture [111,112]. Many types of short fibers including metallic, polymeric, natural and
carbon are used to reinforce the concrete for achieving enhanced properties. Earlier studies [113,114]
on fiber reinforced cementitious composites showed an appreciable inhibition of crack propagation,
thus contributing to the easy crack healing in the concrete. It was concluded that the inclusion
of fibers in the concrete matrix can enhance their engineering properties. Some studies [113,114]
evaluated the feasibility of fiber-reinforced concrete as immobilizers wherein self-healing agents such
as bacteria were used. Rauf et al. [114] showed that natural fibers (coir, flax, and jute) can be used
to carry bacterial spores for self-healing of the concrete. For this purpose, the calcite precipitation
bacteria, namely Bacillus subtilis KCTC-3135T , Bacillus cohnii NCCP-666, and Bacillus sphaericus
NCCP-313, were included in the concrete matrix along with the calcium lactate pentahydrate and urea
as the organic nutrients. It was found that natural fibers are capable of substantial immobilization of
bacterial spores. In addition, the flax fibers provided a better protection to the bacteria with improved
crack-healing and regained compressive strength.
Figure 9 shows the microstructure of three selected concrete specimens incorporated with the
bacteria and natural fibers (B. subtilis with jute (Figure 9a–d), B. cohnii with flax (Figure 9e–h), and
B. sphaericus with coir fibers (Figure 9i–l)). As a carrier, the flax fibers provided a better protection to
the bacteria, indicating an efficient crack-healing and pore-filling ability. Zhu et al. [115] developed
some sustainable engineered cementitious composites (ECCs) by incorporating limestone calcined clay
cement and polypropylene fibers. The results showed that the proposed concrete can attain an efficient
recovery of the composite tensile ductility and ultimate tensile strength through the self-healing
Figure 9 shows the microstructure of three selected concrete specimens incorporated with the
bacteria and natural fibers (B. subtilis with jute (Figure 9 a–d), B. cohnii with flax (Figure 9 e–h), and
B. sphaericus with coir fibers (Figure 9 i–l)). As a carrier, the flax fibers provided a better protection
to the bacteria, indicating an efficient crack-healing and pore-filling ability. Zhu et al. [115] developed
some sustainable
Biomimetics 2020, 5, 47 engineered cementitious composites (ECCs) by incorporating limestone calcined 14 of 22
clay cement and polypropylene fibers. The results showed that the proposed concrete can attain an
efficient recovery of the composite tensile ductility and ultimate tensile strength through the self-
mechanism. It was established
healing mechanism. that the
It was established inclusion
that of fibers
the inclusion in theinself-healing
of fibers concrete
the self-healing matrix
concrete can
matrix
positively affect the mechanical properties and self-healing efficiency of the studied concretes.
can positively affect the mechanical properties and self-healing efficiency of the studied concretes.
Figure 9. (a–l)
(a–l) The
The SEM
SEM image of the healed specimens prepared with different
different types
types of
of fibers
fibers [114].
[114].
7. Self-Healing Evaluation Methods

Diverse tests and techniques have been devised to assess the efficiency of different self-repair
mechanisms. Several factors that determine the capability of crack repair include the width and age of
cracks and type of curing [116,117]. In most studies, microscope-based visual observation is employed
to establish the nature of the wide sealed cracks [37,118]. Other approaches for crack detection include
digital imaging, extremely pixelated camera photographs, and X-ray computed tomography [119].
Meanwhile, the quality of the hardened concrete is assessed via structural tests at the macro-, micro-,
and nano-level. Chloride penetration, porosity, and nano-mechanical value tests can provide an insight
into the self-repair performance. Some studies examined the self-repair capability of the encapsulated
sodium silicate, colloidal silica, and tetraethyl orthosilicate where evaluations were made through
the sorptivity and gas permeability tests [120], revealing a decrease in the sorptivity of 18% and gas
permeability of 69%. Furthermore, the repair material performance has been appraised by Granger
and Loukili [121] via a stiffness test. Farhayu et al. [122] showed the doubling of flexural strength in
the repaired concrete compared to the control sample. Snoeck et al. [123] revealed the deposition of
a white material in the crack via thermogravimetric analysis. Additional tests were undertaken in other
studies to determine porosity and pore size distribution, chloride penetration, and oxygen profile.
Self-repair is considered to restore the compressive strength in a proportion of as much as 60% and
it has also been reported to improve ultrasonic pulse velocity. Consequently, taking into account the test
results, the strategy of biological self-repair could be beneficial for long-term durability, prolonging the
use life of concrete infrastructures. Conversely, not much attention has been paid to additional key
tests, including the strength of bonding between the materials deposited in the cracks and the actual
concrete, the stress–strain relationship curve, and gas permeability tests. As such, different approaches
should be adopted in assessing the capability of concrete self-repair. In short, a more comprehensive
understanding is required regarding the materials’ deposition capacity for binding in the cracks and
their structural compatibility with the components of the concretes.
Micro-tensile, bending and bulge tests were carried out to evaluate the concretes’ mechanical
performance at the micro-size or smaller. Ghidelli et al. [124] stated that the nanoindentation test can be
useful to evaluate the materials’ mechanical properties such as the elastic moduli and residual stresses
because they can provide high resolution in the load and displacement. Diverse methods such as
the micro-pillar splitting approach and micro-cantilever bending are adopted to evaluate the fracture
toughness of the materials in the micro to nano-scale [125]. These methods can potentially be used to
assess the self-healing performance of cementitious materials for achieving better understanding of the
mechanism of self-healing, especially for materials at the nano-scale.
8. Effect of Addition Self-Healing Agents on Concrete Properties

It is established that inclusion of self-healing materials in the concrete matrix can offer several
advantages/disadvantages to the mechanical properties depending on the nature of the materials and
self-healing process. It was found insertion of the capsules in the concrete matrix can result in voids or
holes in the concrete after releasing the contained agent. These voids in turn can negatively affect the
strength performance of the concrete [15]. The use of bacteria spores as the self-healing agent in the
concrete was shown to reduce the compressive strength performance with loss in strength between
8 to 10%. In addition, the loss in strength increases with the increase in bacteria dosages [15,59].
The observed strength reduction was attributed to the microstructure’s alteration induced by the
reduced degree of hydration and poor distribution of the hydration products because of the inclusion
of nutrients and microcapsules. Algaifi et al. [126] reported that the inclusion of microbial calcium
carbonate in the self-healing concrete matrix can improve the compressive strength when compared
with the normal concrete specimens. Similar results were obtained by Shaheen et al. [127] wherein the
mechanical properties of the prepared concrete such as the compressive strength and splitting tensile
strength were enhanced when immobilization techniques for the self-healing process was utilized.
9. Life Cycle Analysis of Self-Healing Concrete

Ample research has been conducted on self-repair technology in the last ten years and its potential
for promoting an autonomous crack healing in concrete has been highlighted. This has led to the
development of several self-repair mechanisms for cementitious materials. The evaluation of various
products and services in terms of their effect on the environment from the moment of development until
discontinuation is based on the life cycle assessment (LCA) methodology achieved standardization as
ISO 14040-14044. In essence, the LCA is geared towards determining whether self-repairing concrete is
more sustainable than standard concrete. Diminished deterioration rate, prolonged use life, decreased
frequency and low cost of repair over the lifespan of a concrete infrastructure are among the main
advantages of self-repairing concrete. These can make concrete more sustainable as reduced repair
frequency translates to a decrease in the amount of material resources and energy used, decrease in
the environmentally damaging emissions associated with the manufacture and transport of materials,
and reduction in the traffic changes to transport infrastructure required by the repair or reconstruction
work [128–131].
Van et al. [132] discovered that chlorides can be prevented from instantly permeating
through the cracks when encapsulated polyurethane precursor was used as self-repair material.
Furthermore, the levels of chloride in an area with the cracks was decreased by at least 75% in the
self-repairing concrete. Compared to standard concrete that has a use life in marine environments
of just seven years, concrete with self-repair capabilities is usable in such environments for about
60–94 years. Lengthening of the lifespan was the main determinant of significant environmental
advantages (56%–75%) according to the computations of life cycle evaluation.
10. Conclusions
In recent times, the production of sustainable concretes via self-healing technology became
useful in construction industries worldwide. The exponential increase in the usage of the OPC
caused severe environmental damages. The immense benefits and usefulness of self-healing concrete
technologies were demonstrated in terms of their sustainability, energy saving traits and environmental
affability. The foremost challenges, current progress and future trends of smart technology enrooted
self-healing concretes were emphasized. An all-inclusive overview of the appropriate literature on
smart material-based self-healing concretes allowed us to draw the following conclusions:
i. Self-healing concretes are characterized through several significant traits such as low pollution
level, cheap, eco-friendly, and elevated durability performance in harsh environmental conditions.
These properties make these concretes effective sustainable materials in construction industries.
ii. The internal encapsulation and hollow fiber-activated self-healing strategies are efficient for
multiple-damages repair. However, these two strategies encounter some complexity in casting
and have a negative impact on the mechanical properties of the proposed concretes.
iii. The inclusion of expansive agents and mineral admixtures in the concrete demonstrated superior
efficiency in the self-healing process. However, it is not very effective in the presence of
multiple damages.
iv. The design of the nanomaterial-based self-healing concretes with improved performances
and endurance are useful for several applications, thanks to the advancement of nanoscience
and nanotechnology.
v. The environmental pollution can considerably be reduced by implementing the high strength
and durable cementitious composites fabricated using diverse nanoparticles, carbon nanotubes
and nanofibers.
vi. In the domain of building and construction, production of materials via the nanotechnology
route is going to play a vital role in sustainable development in the near future.
vii. Use of smart materials in concrete is advantageous in terms of the improved engineering
properties of the cementitious materials, especially for the generation of self-healing and
sustainable concretes.
viii. This comprehensive review is believed to provide taxonomy to navigate and underscore the
research progress toward smart materials based self-healing concrete technology.
Author Contributions: K.W.S., Supervision; G.F.H., writing the original draft. All authors have read and agreed
to the published version of the manuscript.
Funding: This research received no external funding.
Conflicts of Interest: The authors declare no conflict of interest.
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article distributed under the terms and conditions of the Creative Commons Attribution
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biomimetics

Keywords: concrete durability; climate change; sustainability; self-healing technology

Biomimetics 2020, 5, 47; doi:10.3390/biomimetics5040047 www.mdpi.com/journal/biomimetics

2. Concrete Performance in Aggressive Environments

Biomimetics 2020, 5, x FOR PEER REVIEW 4 of 21

5.3. Bacteria as Self-Healing Agent

NH2 COOH + H2 O → NH3 + H2 CO3 Path II

H2 CO3 + H2 O → HCO3 − + H+1 Path III

2NH3 + 2H2 O → 2NH4 + + 2OH−1 Path IV

HCO3 − + H+1 + 2NH4 + + 2OH−1 → CO3 −2 + 2NH4 + + 2H2 O Path V

Ca+2 + Cell → Cell-Ca+2 Path VI

Cell-Ca+2 + CO3 −2 → Cell-CaCO3 Path VII

Biomimetics 2020, 5, x FOR

Figure 8.8. (a) The

5.5. Shape Memory Materials as Self-healer

5.7. Engineered Cementitious Composite

5.8. Nanomaterials Based Self-Healing Concrete

6. Self-Healing in Fiber-Reinforced Concrete

7. Self-Healing Evaluation Methods

8. Effect of Addition Self-Healing Agents on Concrete Properties

9. Life Cycle Analysis of Self-Healing Concrete

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