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1 s2.0 S2352710218310994 Main
1 s2.0 S2352710218310994 Main
1 s2.0 S2352710218310994 Main
Cement industries that produce the main constituent of concrete remain the foremost concern to the world in terms of contributor for
climate change and hindrance towards sustainability. Apart from USA, the fast-developing nations such as China, Indonesia, India, and
Turkey are also causing major environmental pollution. According to Robert Hutchinson (2016), above 4 billion metric tons of OPC that is
produced annually from numerous cement industries worldwide as basic constituent of concrete are primarily responsible for the major CO 2
footprint [1–4]. Identifcation satisfactory and realistic alternatives are challenging task. In the civil engineering sector, OPC is broadly used
as efcient binder in concrete and other construction materials. Meanwhile, OPC manufacturing is commonly accepted as the main provider
of emitted greenhouse gases in the atmosphere [5–8]. International Energy Agency (IEA) reports suggest that it amounts to 6–7% of total
CO2 emissions [8–11]. By the year 2050, the worldwide demand of OPC is expected boost to nearly 200% [8]. Mitigation of CO2 emissions
from OPC related activities requires new types of sustainable, smart and environmental afable self-healing materials [12,13].
It is known that cement materials have very low resistance to aggressive environment and that is one of the most severe problems
afecting the durability and service life of concrete structures in the natural climate. The efect of aggressive environment can manifest in the
form of expansion and cracking of concrete. Sometimes the cracking of concrete may cause serious structural problems [14,15]. In this
sense, the continuous increase in the durability requirements of the concrete structures led to the development of smart concretes (using self-
healing technology) where excellent durability is mandatory [16]. Generally, self-healing is benefcial for the materials’ durability.
Particularly, it is advantageous when human interference is difcult such as in construction purposes in the midst of harsh physical and
chemical environments. Self-healing is also required to protect material characteristics especially in kinetic and thermodynamic conditions
that support large defects density like nanostructures. Nanomaterials invariably reveal excellent functional attributes. Compared to ordinary
materials, nanomaterials degrade faster due to the presence of numerous interfacial atoms. Many functional nanostructures can be combined
to fabricate diverse nanosystems, wherein some components can also be incorporated to ofer self-healing actions. In fact, this strategy is
simplistic compared to the design of a more robust nanosystem [17]. Of late, due to the rapid advancement of nanoscience and
nanotechnology the design and fabrication of self-healing materials has taken new frontiers, wherein materials with particle size below 500
nm is termed as nanomaterials. Self-healing materials can recover from the damages autonomously. In many circumstances, the self-healing
action can also be prompted via temperature as external stimuli, systems with this capacity are called non-autonomic self-healing materials
[18].
Looking at the future prospects self-healing concrete, this communication revisits the ongoing research activities on nanomaterials based
self-healing concrete benefcial for future sustainable developments. Present paper is organized in three main sections. Section 1 discusses
⁎
Corresponding authors.
E-mail addresses: fhghasan@utm.my (G.F. Huseien), bdgskw@nus.edu.sg (K.W. Shah).
https://doi.org/10.1016/j.jobe.2019.01.032
Received 18 September 2018; Received in revised form 25 January 2019; Accepted 25 January 2019 Available
online 26 January 2019
2352-7102/ © 2019 Published by Elsevier Ltd.
G.F. Huseien et al. Journal of Building Engineering 23 (2019) 155–171
the importance of self-healing concrete towards more sustainable and smarter growth in the building sectors than the existing traditional
concretes in terms of enhanced environmental friendliness and pollution reduction. Second section highlights some undertaken strategies of
self-healing processes that disclosed repairing mechanisms with sophistication, elegancy and efciency. Various mechanisms of selfhealing,
benefts and drawbacks of every strategy are emphasized and compared. Section 3 deals with based self-healing systems as feasible solution
of self-recovery mechanisms when active concretes are exposed to corrosion, deterioration, degradation and cracking.
Universally, OPC has been continually exploited as concrete binder and diferent building substances. It is known that production of
OPC based concretes needs huge amount of fuel and raw ingredients that are acquired via resource mining and energy exhaustive processing
[9]. This in turn causes great quantities of greenhouse gases (essentially CO 2 and NOX) emission into the atmosphere. Per ton of OPC
manufacturing, almost one ton of CO 2 is created by consuming 2.5 t of raw materials and fuel [19–22]. Some estimates revealed that
approximately 1.35 billion tons of CO2 is emitted per annum from the OPC production industries alone, accounting nearly 7% of the total
greenhouse gases released to the environment [8,23]. Compared to CO2 levels in 2010, the CO2 emissions from OPC industries on the earth's
atmosphere is going to be a major environmental concern because the global demand of OPC is predicted to grow nearly to 200% by 2050
[8]. Over the years, numerous strategies were adopted to reduce OPC manufacturing including the durability enhancement of concrete and
elongation of service lifespan. In this standpoint, self-healing concrete is emerged as one of the gifted solutions to mitigate the OPC
generated environmental pollution. 2.2. Concrete durability
Characteristically, the serviceability of construction materials has considerable economic signifcance, particularly with modern
infrastructures and components. For urbanization, concrete materials that are greatly exploited must meet the standard codes of practices
requisites’ related to strength and durability [24]. For instance, poor plan, low capacity or over-load, faulty material design and structures,
wrong construction practices or unsatisfactory maintenance, and lack of engineering knowledge can often diminish the service life span of
concrete under operation [25]. In the construction industries fast declination of concrete structures being a major setback necessitates
additional improvement. Varieties of physical, chemical, thermal and biological processes are responsible for the progressive deterioration
concrete structures during their service [7,26]. Several studies [27–29] revealed that the concrete performance is greatly afected by
improper usage, physical and chemical conditions of environments. It is verifed that both external and internal factors involving physical,
chemical, or mechanical actions are often responsible for the deterioration of the concrete structures.
Mechanical damage of concrete structure occurs due to diferent reasons such as impact, abrasion, cracking, erosion, cavitation, or
contraction. Chemical actions that cause the declination of concretes are carbonation, reaction associated with alkali and silica, alkali and
carbonate as well as eforescence. Moreover, outside attacks of chemicals happen primarily due to CO 2, Cl2, SO4 as well as several other
liquids and gases generated by the industries. Physical causes of deterioration include the efects of high temperature or diferences in the
thermal expansion of aggregate and of the hardened cement paste. Other reason of deterioration is the occurrence of alternating freezing and
thawing of concrete and the associated action of the de-icing salts. Physical and chemical processes of deterioration often act in a synergistic
way including the infuence of sea water on concrete. Poor durability performance of OPC in aggressive acidic or sulphate (especially in
marine) environment is caused due the existence of calcium complexes. These calcium complexes are very easily dissolved in acidic
atmosphere, leading to enhanced porosity and thus fast deterioration [30].
In many places worldwide, OPC structures that are existing for many decades are facing rapid deterioration [31]. Defnitely, the
permanence of OPC is linked with the nature of concretes’ constituents, where CaO of 60–65% and the hydration product of Ca(OH)2 nearly
25% is responsible for fast structural decay. Several studies indicated that occurrence of fast reaction of Ca(OH) 2 in the acidic surroundings
allows OPC to be deprived of water, leading to acid fusion and weakening of resistance against aggressive attacks. On the top, the intense
reaction of evolved CO2 with Ca(OH)2 contribute to rapid corrosion of the concretes containing OPC [31]. The safety, service life,
permanence, and life span of the mix design of concretes are considerably infuenced by the cracks development and subsequent erosion.
These distinguished drawbacks of OPC based concretes drove researchers to enhance properties of conventional OPC by adding pozolanic
materials, polymer and nanomaterials so that it becomes more sustainable and endurable. The immediate consequence for a fected concrete
structures is the anticipated need of maintenance and execution of repairing [32]. Thus, there is a renewed interest for the development of
sustainable concrete to solve all these existing shortcomings involving harsh environmental conditioning and durability.
Nowadays, cement is the primary workhorse in the construction sectors worldwide. Cement is processed at high temperature ( ≈1450 °C)
in a rotary kiln by mixing limestone or chalks with clay. Next, the yielded hard nodules of clinker are crushed with low amount of gypsum
using ball milling technique. Firing of such cement constituents at higher temperature needs substantial amounts of energy to be consumed
(burning of coal or petroleum coke). Rapid decay of land setting, generation of dust during transport, creation of noise all over quarrying and
processing of raw materials are regarded as major environmental concerns in OPC production. According to previous publications [28,33],
OPC manufacturing devoid of considerable amounts of CO 2 release is impossible. Actually, the CO 2 emission occurs in two phases including
fuel burning (to achieve very high temperatures of klin) and calcining (a chemical reaction occurs during limestone fring). Until now, even
the most efcient cement production plant emits 60% or more of CO 2 from various inevitable chemical pathways. The consumption of a
considerable quantity of energy during crushing of cementitious raw materials in the clinker phase remains the foremost ecological distress
in the OPC industries [34,35]. Undeniably, developing autonomic self-healing cement-based materials must be realized as a practical
solution to the existing problems.
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3. Self-healing concrete
Low carbon emission and energy saving building material incorporated with smart material (in self-healing technology) is a wellknown
candidate energy technology in enhancing energy efciency and sustainability of building. The major aim of sustainable development is to
keep livelihood on earth in the predictable future with absolute support or care so that ecological balance is not disturbed [36]. Sustainability
is founded on three basic elements such as the economic security, environmental safety and societal bene fts. Sustainable advancement must
preserve these factors to protect the biodiversity with balanced ecosystem. In the present industrial uprising era, engineers, scientists,
policymakers and architects are attempting to use resourcefully the sustainable model to reduce the negative impact on our ecosystem.
Therefore, in the perspective of building materials the phrase sustainability used synonymously with robust or friendly and green
environment [37,38]. In this viewpoint, self-healing materials have attracted increasing interest due to their potential to lessen the
degradation, prolong the functional lifespan, and suppress the maintenance costs of materials [39,40]. However, the self-healing technology
contributions directly to enhance the environment and reduction the pollution from increasing concrete life-span and reduction the demand
and consumed of OPC as well ‘as afecting to saving energy and increase the sustainability of concrete.
During the past decade, the self-healing technique extensively studied and introduce as an innovative technique for concrete crack
selfrepair. However, several innovative strategies to self-healing for cementitious materials have been proposed and developed. Nowadays, it
is known as the life cycle assessment (LCA) methodology which has been standardized in ISO 14040–14044. Thus far, it has been used for
assessing the environmental impact of all kinds of products and services preferably from the cradle to the grave. The goal of this LCA was a
quantifcation of the environmental impact reduction that could be achieved by using the proposed self-healing concrete instead of a more
traditional concrete. Some direct benefts of concrete self-healing include the reduction of the rate of deterioration, extension of service life,
and reduction of repair frequency and cost over the life cycle of a concrete infrastructure. These direct benefts may be expected to lead to
enhanced environmental sustainability since fewer repairs implies lower rate of material resource usage and reduction in energy
consumption and pollutant emission in material production and transport, as well as that associated with tra fc alterations in transportation
infrastructure during repair/reconstruction events [41]. Van Belleghem et al. [42] has reported the Self-healing of cracks with encapsulated
polyurethane precursor formed a partial barrier against immediate ingress of chlorides through the cracks. Application of self-healing
concrete was able to reduce the chloride concentration in a cracked zone by 75% or more. Service life of self-healing concrete in marine
environments could amount to 60–94 years as opposed to only 7 years for ordinary (cracked) concrete. However, life cycle assessment
calculations indicated important environmental benefts (56–75%) and mainly induced by the achievable service life extension.
In human body, injured surfaces (skins) and tissues are self-recovered due to the assimilation of nutrients that creates new substitutes to
repair the injured parts. Likewise, in the self-healing of cements based materials essential products (acts as nutrients) are supplied to heal the
cracks in damaged concretes. In the past few decades, intensive investigations have been performed to explore novel strategies for ef fcient
self-healing with durability. Fig. 1 provides a schematic presentation involving the developed self-healing strategies for cementious
materials.
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external and internal diameter of 2 mm and 0.8 mm was positioned within the specimens. Both dilute (27%) non-dilute alkali-silicate
mixture and 2 components combined epoxy resin of low viscosity were utilized for selfhealing component. Subsequently, this complex
solution was loaded until the Crack Mouth Opening Displacement (CMOD) reached to 0.03 –2 mm after the elimination of the load. Next,
these cracked samples were again cured to examine the improvement of self-healing ability. Compared to normal specimens (without
healing agent) specimens that contained the dilute and non-dilute alkaline silica solution as the healing component correspondingly revealed
a mean ratio of the strength recovery of 1.1 and 1.5. Conversely, specimens in the presence of epoxy resin displayed little improvement in
the strength recovery ratio, which was much below the value that was obtained by direct mixing of resin and manual injection into the
cracked regions (about three times better recovery). This observation was majorly ascribed to the inadequate blending and stirring of the two
constituents, which produced the low healing ratio due to less hardening of resin. It could also be due to the presence of some residual epoxy
that remained inside the pipes because of the sealing of one end.
According Joseph [55], the testing regime was analogous except some insignifcant distinctions. Bent plastic tubes with respective
external and internal diameter of 4 mm and 3 mm were employed as the vehicle of healing mediator (Ethylcyanoacrylate). It was concluded
that supply of such healing component externally could achieve self-healing successfully. After healing of the damaged area the stifness
after crack, the peak load and the ductility were enhanced considerably. Results during and after test revealed that, ethyl cyanoacrylate as
adhesive could penetrate a large area of the fractured surfaces due to the
3.3.2. Microencapsulation
With the time, the man-made materials for encapsulation were developed from natural examples spanning from macro- to nano- scale.
Birds’ egg or seeds are the simplest illustration of natural encapsulation on a macroscopic scale and a cell within it is an example on
microscopic scale [57–59]. The growth of microencapsulation started with the synthesis of capsules comprised of dyes, which was then
included in paper for the copying and replacing the carbon-paper [60]. Over the passage of time, several novel technologies have been
developed in diverse areas. Microencapsulation is not considered as disconnected product or part of it, which is rather de fned as the
development of including micrometer size solid granules or liquid drops or gases within the inert shell, isolating and protecting them from
unnecessary reactions in the outside surroundings [61,62]. The implementations of microencapsulation with self-healing products were
established [61,63]. Fig. 3a explains the self-healing idea, where the crack ruptures the implanted microcapsules, resulting in the release of
healing agent into the crack surfaces via capillary action. Thereafter, the healing agent comes in contact with the embedded catalyst,
inducing polymerization and thus closing of the surrounding cracks. Fig. 3b displays a typical cracked microcapsule image.
Nishiwaki [64] reported the flling of microcapsules using epoxy resin as healing material where the shell of urea–formaldehyde
formalin in the size range of 20–70 µm was incorporated. These microcapsules plus acrylic-resin (an hardener in the form of gelatin shell of
size range of 125–297 µm) were employed. It was shown that
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Fig. 3. (a) The microcapsulation approach and (b) typical ESEM micrograph of a cracked microcapsule [61].
microcapsules incorporated with sodium silicate were efective for investigation of agents [69,70]. A comparison of the reference
selfhealing [65]. In this work, concrete was frst stacked to almost specimen was made with the specimen containing 10% cement
the breaking point before the load was removed and then cured for substituted by expansive materials comprised of C 4A3S, CaSO4 and
1 week. Results revealed the concrete with 2% sodium silicate CaO (lime) was conducted. It was revealed that for concrete beams
microencapsulation could recover as much as 26% of its actual containing expansive agents could almost heal the presence of an
strength compared to the reference sample (recovery of 10% only). early crack of 0.22 mm later than 1 month, in which rehydration
It was concluded that by growing the healing material's amount yield among cracks was identifed. Nevertheless, for the ordinary
even upper strength recovery ratio could be attained. Jianying Yu concrete structure these cracks were partially healed during the the
et. al [66] inspected the one-component microcapsules were same time period. Therefore, re-crystallization of expansive agents
prepared with toluenedi-isocyanate (TDI) as the healing agent and in air voids for selfrecovery was extra efcient compared to normal
parafn as the shell. The results indicted d that the TDI was concrete [67]. Tanvir Qureshi et. al [29] reported that the expansive
successfully encapsulated in the parafn shell and The mortars with minerals improved the self-healing capacity of concrete mixes. The
the microcapsules showed more favorable self-healing capacity. autogenous self-healing performance of any particular cement mix
could be numerically predicted based on their hydration degree
3.3.3. Expansive agents and mineral admixtures which is an indicator of cement mix state at any particular age.
Kishi et al. [67] reported the creation of cementitious materials It was also demonstrated that a geo-material containing SiO 2
such as Al2O3–Fe2O3-tri (AFt), Al2O3–Fe2O3-mono (AFm) and (71.3%) and Al2O3 (15.4%) when added to the expansive material
calcium carbonate (CaCO3) in the cracked concrete and air voids of could form a geo-polymer via polymerization of aluminate and
Ca(OH)2 crystals. It was assumed that such hydration yields could silicate compleaxes individually [68]. Subsequently, these were
leached out and re-crystallize in the fown water through the dissolved at high pH due to the existence of alkali metals.
Thorough investigation revealed that the size geo-polymer gel
fractures. According to this idea, Kishi and co-workers [67–69]
particles were below 2 µm and the cracked interfacial phases of the
evaluated the self-healing concrete performance with diferent
original ruptured zone generated numerous hydro-garnet or AFt
healing agents. Expansive agent, geo-materials and chemical
mixtures together with their blends were included in the
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phases (Fig. 5). Thus presence of expansive agent played a decisive ions (Path III and IV). Path IV and V was responsible for the
role to bridge those cracks. enhancement of pH, drifting the bicarbonate equilibrium to form
carbonate ions.
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the mortar beam containing SMA wires could recover about totally agents such as water and salts from coming in contact with rebar.
after sustaining a very huge crack. Likewise, shape memory The development of polymer coatings that react to environmental
polymers (SMPs) have been developed by Jeferson et al. to stimuli such as heat or pH changes to initiate crack healing has also
incorporate into cementitious materials [79]. When crack arises in been investigated [91,92]. Coatings that react to heat have achieved
the cementitious matrix because of early age shrinkage, thermal success, with some retaining all of their mechanical properties after
infuences and/or mechanical loading then the shrinking process in multiple healing cycles [93]. As polyelectrolyte nanocontainer
the included SMA tendons can be stimulated by heating. This in coatings, changes in the pH of the solution have been able to set a
turn can repair the cracks by developing a measurable compressive response within seconds [94]. Full recovery of the mechanical
stresses across the closed crack surfaces. Such cracks closing properties of the coatings were also achieved, making it a
mechanism can improve the natural self-healing processes and the promising option for research in the future [94]. Drying oils such
durability performance of the structural elements in concrete. It as tung oil and linseed oil have received signifcant investigation
was concluded that post-tensioned mortar beams via aligned regarding their healing properties and encapsulation [95–97]. When
shrinked polymer tendons could be efective for crack closing and exposed to air, tung oil will polymerize into a tough, glossy,
weak prestressing. Results from several screening tests revealed waterproof coating. These characteristics have made drying oils a
that the most efcient tendons were polyethylene terephthalate valuable component in paints, varnishes, and printing inks. Tung
(PET) Shrinktite with a shrinking potential of about 34 MPa at oil encapsulation was frst achieved by Samadzadeh et al. [98].
controlled situations with 90 °C heating and subsequent cooling These urea-formaldehyde microcapsules displayed good adhesion
down to room temperature. The infuence of heating together with to the epoxy matrix, compared to industry standards, by testing the
extra curing could enhance the mortar's strength around 25%. microcapsules pull-of strength following ASTM D4541-09.
Testing of damaged samples to measure service life through
3.3.6. Coating immersion in sodium chloride solutions was conducted. Results
Recent developments in materials’ technology provide extra were promising, as the tung oil microcapsules extended service life
functionalities leading to the term of “intelligent material” which up to nine times that of epoxy coatings after damage.
are characterized via desired response to some external stimuli
such as temperature, light, humidity, etc. Innovative materials for 3.3.7. Engineered cementitious composite
buildings (coatings) have been developed and tested successfully In the early 1990s, the special class of concrete called ultra-
[84,85]. Amongst these materials we may fnd coatings for self- ductile fbre reinforced cementitious composites was designed.
healing concrete with specifc durability properties. The technical Originally, it is known as Engineered Cementitious Composite
of self-healing coating used with reinforcement concrete for steel (ECC) [99], which is constantly improved over the last two decade
bar self-healing and reduction the corrosion damaged. Self-healing [16,99]. This material possesses high ductility (3–7%), tight crack
coatings are a recent avenue of research that could provide a way size (about 60 µm) and comparatively low fbre content (roughly
to fght the deterioration of modern infrastructure. Conventional 2% or lesser by volume) [100]. Actually, metal-like feature is the
anti-corrosive coatings have limited effectiveness if even a small signifcant mechanical character of ECC. It can sustain elevated
portion of the coating is damaged [86]. Selfhealing coatings, loads after initial crack during auxiliary distortions. Li et al. [101]
however, can continue to function due to their ability to heal after examined the self-repairing idea of Dry [52] related to bleeding
fracture [87]. In efect, this self-repair is anticipated to be able to which was used to discharge chemicals that could close the tensile
greatly prolong the life of steel rebar structures. Initial cracks with subsequent air curing. This mechanism led to regain
investigation into application on steel rebar was conducted by Chen the mechanical properties of the un-cracked composites. It was
et al. [88]. This technology could be applied to rebar structures that acknowledged that the self-healing process was inefective for
are typically coated with epoxy coatings in the highly corrosive usual concrete, cement or concrete reinforced with fbre. It is due
areas of the Northeast to combat rapid corrosion rates. the difculty in controlling the size of the tensile cracks in these
In the past, many studies have been conducted [12,13,26] to materials. Local breakages could multiply continuously inside the
determine the mechanism of protecting the concrete roads, bridges crack width under declining tensile load and exhaust quickly the
and other structures against tiny cracks development. Yet, no accessible chemicals responsible for crack closure and re-healing.
conclusive remark has been made and thus remained as major Therefore, effective self-recovery requires the control of the tensile
issue. Cracks allow water, salt used for deicing and air to enter the crack width which must be restricted within tens of micros. Else,
concrete. During winter season, frozen water inside the cracks very large glass pipes are needed to modify the mechanical
expands and made them bigger, speeding up concrete's characteristics of composites. This argument was consistent with
deterioration in the presence of road salt. Many investigations have several other reports, that emphasized the role of cracks width
been conducted on self-healing anticorrosive coatings for [102–104].
protection of metals but no work is performed on self-healing The tightly controlled crack size being one inherent
protective coating for concrete. Self-healing coatings that initiate characteristics of ECC can ofer advantages for applying the self-
selfhealing through external cracking or damaging has seen healing idea to ECC. Later, two diferent experiments were
substantial research. These coatings often have micro containers conducted [30] to examine the viability of the proposed bleeding
mixed in that can rupture easily when acted upon. The containers notion. In the frst experiment, the ECC materials with a single
hold healing agents that then seal the crack and prolong the empty glass fbre free of any healing chemical were tested in situ at
functionality of the coating. Containers that hold these healing
a loading stage under an FESEM. The idea was to confrm the
agents can vary from polyurethane microcapsules to microflament
sensing and actuation properties of ECC. The other experiment was
tubes and often have little efect on the mechanical properties of performed to measure the fexural strength of ECC containing the
the coating. Research in this area has provided good results and
glass fbres packed with sealing material (ethyl cyanoacrylate).
application in real world environments can be further investigated
Both studies were performed under MTS load-frames to ascertain
[87,89,90].
the re-healing efectiveness of the sealing mediator after sustaining
Many types of organic and inorganic materials used for this
damage (fracture) in the load-cycles. The sensing and actuation
purpose. Epoxy coatings are widely used to prevent corrosive
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processes were authenticated using FESEM images and the the self-recovery process. The signifcance of crack size was
infuences of revitalization were authenticated via fexural stifness underscored in the context of constant hydration dependent self-
regain. It was also acknowledged that several other issues need recovery because it consumed very low amount of healing
further investigation before practical applications could be made. materials to close the cracks and was easy for the healing
Li et al. [50,105,106] also examined the self-healing phenomena of specimens to develop from both faces of the cracks for joining.
cementitious materials in addition to the inclusion of external Commonly, the micro-crack behaviour and the cracking chance
chemical as healing glue in concrete. The concrete matrix and its of ECC in the presence of micro-encapsulated modules were found
interaction with the exposed surroundings were examined. The to improve, wherein healing materials were released. This assured
ECC specimens were precracked and exposed to various the efciency of the sensing and actuation processesthrough micro-
environments such as water permeation and submersion, cycles encapsulation. The tight crack size in ECC is greatly signifcant
related to wetting and drying, and chloride ions attack. Results because it needs low quantities of healing products for cracks
revealed that the mechanical and transport characteristics was flling and efcient for the healing products to develop from both
principally recovered, particularly for ECC preloaded with tensile facades for connecting these cracks. In short, ECC possesses higher
strain below 1%. Apart from the tiny cracks, the small water/ fraction of cementitious materials and lesser water to binder ratio
binder ratio and the presence of great quantity of FA in the mixture than conventional cements, thus more efective self-healer. Table 1
could support the self-recovery action through hydration and enlists the benefts and drawbacks of various self-healing concrete
pozzolanic mechanisms. strategies developed in the past.
The ECC materials was locally developed from waste matters
and/or by-products [107]. Several mixtures were designed using 4. Nanomaterials
powders of blast furnace slag (BFS) as well as limestone (LS) and
subsequently analyzed by measuring the tensile strain (2–3%) as 4.1. Production of nanomaterials
well stif cracks (with typical size < 60 µm). It was found that [108]
the mixes designed by Zhou et al. [107] were dissimilar from the It is well known that nanoparticles produce superior efect on
one casted by Li et al. [50] in terms of basic constituents (high fller than micron-sized materials. Guterrez [123] acknowledged
proportion of BFS and LS instead of FA) and very high water to that all materials can be converted into nanoparticles via crushing
binder ratio in the range of 0.45–0.60 against 0.23. This indicated or chemical treatment. The production accuracy of nanoparticle is
that the quantity of un-hydrated cementitious materials cured later decided by the purity and the chemical constituents of the parent
than 28 days was much below the one used by Li et al. [101]. It materials. Two routes are followed for the large scale production of
was shown that ECC specimens made from great quantity of BFS, nanomaterials including the top-down approach [124] and bottom-
LP and reasonably high ratio of water to binder that could restore up approach [125]. These approaches are chosen based on the
comparable self-repairing properties than ECC materials analyzed appropriateness, price and knowledge of the nanoscale properties
by high proportion of FA and low water to binder ratio. This of the material under consideration [126]. Milling technique fall in
observation was ascribed to the presence of tight crack width, the category of top-down approach, wherein the selection of
wherein the self-healing of ECC was decided by the availability of milling machine is favoured due to its accessibility,
un-hydrated cement and other complementary products including inexpensiveness and feasibility of easy modifcation without
BFS. Therefore, low ratio of water to cementitious material ratio requiring any chemical reagents or complex electronic equipments.
and high fraction of cementitious specimen were useful to support In the top-down approach, big structures (bulk) are transformed
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G.F. Huseien et al.
Table1
Comparisonofvariousself-healingconcretestrategies.
Precursors Products
163
andnatural Measuresmustbetakentoshieldbacteriainconcrete
Mechanicalfeaturesrecoveryandefcacyformanydamagesmaybea
concern.
[117–119] ShapememorymaterialsEnhancedtheetringite C-S-HgelMacro-crackscanbetackled.Expensive
formation StrongrecoveryinthemechanicalbehaviourInductionofealingviaheatreatmentleadstouncertainties.
Efectivenesstowardsmanydamagesevents
[120] CoatingMethodPolymerReductionthe EasyMaintenanceManyprerequisitestobemet.
EpoxyCheap porosity
DecreasethecorrosionproblemsE fciencytowardsnumerousdamagesmaybeasetback
Forexternalhealing.
[121,122] NanomaterialsSiO 2,Al 2O3 C-(A)-S-HgelsStrongrecoveryinthemechanicalbehaviourHighsafetyrequirements.
TiO2,Fe 2O3 EfectivenesstowardsmanydamagesForinternal
andexternalapplication
Cheapandsavingenergy.
Excellenthealingefcacy.
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G.F. Huseien et al. Journal of Building Engineering 23 (2019) 155–171
to small one (nanodimension) while keeping their actual physical cement hydration process and pozzolanic reaction, reduction of
or chemical behaviour intact via atomic level control [127], which pores density, and enhanced interfacial bonding amid hardened
has been applied at industrial level. Using milling technique, high cement paste and constituents (aggregates). Nanomaterials were
volume of nanoparticles can be produced. Though top-down also exploited to reduce the porosity and enhance the durability
approach is contemporary for nanofabrication, the consistency and properties of concrete [137,138]. With developing the concrete
superiority of the yields are often unpredictable. To overcome such technology, the nanomaterials were used in many applications (Fig.
drawbacks, the milling techniques (a top-down approach) can 5) and the self-healing technology one of the important application
further be improved by increasing the number of balls, ball types, to produce sustainable and smart concrete.
milling speed, and nature of the jar, where the quality of
nanoparticles become better [128]. 4.3. Production of nanoconcrete
High energy ball milling technique has been widely used to
fabricate diverse nanomaterials such as nanoparticles, nanograins, Using materials with a particle size less than 500 nm in
nanoalloy, nanocomposites and nano quasicrystals. John Benjamin concrete production as admixture or part cement replacement
introduced this technique to produce oxide particles inside the called nanoconcrete. It was shown that the strength of normal
matrix of nickel superalloys (1970). Utilizing milling technique the concrete tend to enhance with the inclusion of nanoparticles. The
properties of alloy component efective for high thermal structure bulk properties and packing model structure of concrete can
was altered and mechanical strengths were improved. Factors remarkably be improved via the incorporation of nanoparticle.
including fractures, plastic distortions/deformations, and cold Nanoparticles act as excellent flling agents through the refnement
welds during the milling process afect the materials conversion of intersection zones in cementitious materials and production of
into the desired morphology. Milling not only crushes the material high density concrete. The manipulation or modifcation of these
into tinier fragments but also blends numerous particles or nanoparticles in the cement matrix can render a new-fangled
materials to transform into new phases with diferent compositions. nanostructures [139–141]. General defciencies in the
Usually, the fnal yields of milling technique are in the form of microstructures of concretes including voids, micro-porosity and
fakes where refnements are performed based on the selected ball corrosion originated from the reaction of alkaline silica can be
and milling standard. Most of the nanomaterials (nanosilica, nano discarded. The advancement of nanomaterials occurred due to their
alumina, nanoclay) utilized in concrete can be obtained via bottom- characteristics as new binding agent with particles sizes much
up approach, which is adopted for materials engineering at atomic tinier than traditional OPC. This property enhances the hydration
or molecular levels via the self-assembling process so called gel product by imparting a neat and solid structure. Besides, using
molecular- nanotechnology or molecular-level processing. It is a blend of fller and extra chemical reaction in the hydration
applied indirectly in nanomaterials and chemical production [32]. scheme, high performing novel nanoconcrete with enhanced
Varied morphology of nanoparticles obtained via bottom-up durability can be achieved.
strategy is often customized through chemical synthesis technique. The application of nanotechnology in concrete is still in its
In comparison to top-down strategy, the bottom-up strategy can infancy. Ever-growing demand for ultra-high performance concrete
generate nanomorphology with more uniformity and (UHPC) and recurring environmental pollution caused by OPC
reproducibility. Besides, using bottom-up approach one can enforced the engineers to exploit nanotechnology in construction
produce novel nanocrystals with perfect atomic or molecular materials. Classical blends of UHPC with incorporated silica fumes
ordering. Bottom-up approach based production of nanomaterials can achieve enhanced strength and high durability. However,
are useful for achieving high electronic conductivity, optical limited accessibility and highpricing of nanomaterials not only
absorption and chemical reactivity [129]. Through bottom-up slowed down the growth of UHPC technology but also made it less
strategy, one can get tinier size and formation of consistent surface demanding compared to conventional high strength concrete
atoms with modifed surface energies and morphologies. Usually, (HSC). To overcome these limitations, nanotechnology enrouted
bottom-up technique is exploited to prepare self-healing and production of UHPC emerged in its own right wherein an
selfcleaning nanomaterials with improved catalytic properties, alternative to silica fume has been developed. Exploiting the
sensing capacity and novel pigments characteristics. Moreover, the nanoproduction idea, a typical nanomaterial mimicking the
main drawbacks of bottom-up scheme is related to high running attributes of silica fume was designed. Nanosilica is certainly the
cost, need of experts for chemical synthesis and limitation to newest material in nanotechnology based processing that has been
laboratory orientation only [130]. The nanoparticles produced used as substitute to silica fume [142]. Using this celebrated
using bottom-up approach is excellent for advance applications nanosilica component, several types of nanoparticles have been
including electronic components and biotechnology. synthesized which are efective for concrete production [143],
Nanoalumina [144],titanium oxide nanoparticles [145], carbon
4.2. Nanomaterials based concretes nanotube [146] and nanopolycarboxylates [147] are the emergent
nanomaterials in the new nanoconcrete era. It is now customary to
In recent years, the growth in nanotechnology and the discuss about the production and possible applications of
accessibility of nanomaterials suited for construction usage nanomaterials.
including nanosilica, nanoalumina, Polycarboxylates and
nanokaolin have improved the concrete properties remarkably 4.4. Signifcance of nanomaterials as self-healer
[126,131,132]. Intensive researches revealed that the mechanical
properties such as compressive strength, splitting tensile and The contribution of nanomaterials in enhancing the workability,
fexural strength of cement pastes [133,134], mortars [131,135], strength and durability of building materials can afect the
and concretes [136] can be improved via a tiny quantity of hydration kinetics of cement. Furthermore, the addition of
nanomaterials. Early strengths of pastes, mortars [131,135] and nanomaterials can improve the performance of cement appreciably.
concrete [136] in the presence of nanomaterials were reported to be The high performance of nanomaterials attracted the researchers to
much higher than those formulated with conventional OPC. apply nanomaterials to create sustainable concrete by self-healing
Development of such higher strengths were ascribed to the faster technology. The demerits of preceding methods are used for self-
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healing such as tricky to harden the bi-components healing system. inside the concrete, leading to dense and refned micro-voids to
The amount of healing materials packed inside the microcapsules impart smart microstructures [154]. Other benefts involving
was little. Strength of bonds amid the microcapsules and the nanosilica is the better control of water to cement ratio, wherein the
cement network required to be stronger than that of the former. It strength can be customized easily. Quercia. et al. [155] reported the
led the researchers to resolve these problems and fnd another way incorporation of nanosilica at certain dosage improved the strength
to produce sustainable concrete with performance. In order to solve of concrete and performed as cement substitution component.
these problems, the merits of nanomaterials are presented in a Nearly 20–30% of cement could be lowered via the
nowadays, make the researchers in this feld believe to these implementation of nanosilica, thereby it can be a good substitute to
materials will be the best way for sustainable concrete. cement. In self-healing application, the capacity of nanosilica to
react with available Ca(OH)2 in concrete and formulate (CSH gel)
5. Nanomaterials based self-healing concrete was examined [156–159]. Using nanosilica the self-healing
concrete technology as additional mineral admixtures or in
Advancement of self-healing materials in concrete industries is an nanoencapsulation method has been studied. However, the
emerging trend. The generic term self-healing concrete is used for disadvantage of nanosilica is the cost and availability in certain
cement-based materials that repair themselves after the material or nations where nanosilica need to be imported for usage in the
structure gets damaged via diverse deterioration mechanism. concrete industries [32].
Nowadays, using nanomaterials for sustainable concrete also gets a
lot of attention around the world. Compound the two technologies
5.2. Nanoalumina
(selfhealing and nanomaterials) together contributed to enhancing
the durability of concrete and successfully led to producing
In the cement hydration, it is known that the silica and alumina
sustainable concrete [148,149]. Most application of nanomaterials
are two main components involved to formulate C-(A)-S-H gels
in self-healing has been used to control the corrosion of steel bars
with calcium. The role of silica inside cement was to alter strength
in reinforcement concrete. Koleva [148] have been reported the
whereas alumina controlled the setting-time. Nanoalumina is
ability to Improving reinforced concrete performance by
produced from alumina, where the use of nanoalumina in concrete
incorporating nanoscale materials with tailored properties i.e. core-
is seldom reported. The inclusion of nanoalumina in concrete
shell polymer vesicles or micelles in the cement-based system. Few
researches have been conducted to using nanomaterials for self- particularly high performance concrete can enormously afect
healing concrete. concrete characteristics because it regulates the setting-time of
Qian et al. [150] studied the curing situations in the presence of cement [161,162]. Presence of nanoalumina within cement can
air, CO2, and water in the wet-state as well as dry-state. accelerate the early setting-time for high performance concrete,
Furthermore, the efects of nanoclay with water (used as inner which in turn diminishes the segregation and focculation. In high
water furnishing agent for hydration) on the micro-cracks were performance concrete mixes, any disturbance in the cement creates
determined. Results revealed that the healing extent could be inhomogeneity and afects the working performance. Nanoalumina
considerably superior with the inclusion of nanoclay and better in high performance concrete functions as dispersive mediator in
cementitious materials concentration for mixes. It was stated that cement particulates [163,164]. Besides, nanoalumina can refne the
for all studied air cured mixtures, the fnal crack did not occur at porosity of hydration-gel product as nanofller because the cement
the new location, indicating good healing. Despite the interior proportion in high performing concrete is high. Therefore, grains
water supply from nanoclay it revealed comparatively weak size distribution in such concrete is essential simultaneously with
strengthening, enabling it hard to relocate the fnal crack-sites from silica mediated hydration. Without nanoalumina mediated
pre-existing one to another positions. This unproductive recovery refnement, the hydration mechanism is weaker since the silica
with air curing was also reported by Hua [63]. It was shown that component cannot penetrate the interior structure of the gel.
the self-healing behaviour of ECC with Super Absorbent Polymer Incorporation of nanoalumina can create a path for easy injection
(SAP) capsules with water as the interior pool for extra hydration of the silica or binding materials into the interior microstructures of
was efective. Meanwhile, various repairing products were the hydration gel to start the refnement [165,166]. All these merits
recognized across the cracked facades. However, noticeable healed are mentioned above make the nanoalumina one of the important
cracks were absent completely. It was acknowledged that the materials can use in future to produce smart and sustainable
cracks could very likely undergo via the self-recovery mechanism concrete by using self-healing and nanotechnology.
without much efectiveness. The signifcance of enough water or
moisture accessibility was highlighted that acted as the reactant for
additional hydration as well as the ions transportation media.
5.1. Nanosilica
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5.3. Carbon nanotube oxide group provides a non-uniform electron cloud distribution and
chemical polarities to the secondary or side reactions. The number
Carbon nanotube (CNT) is a carbon and the length of secondary or side groups are can easily be
allotrope having cylinder shaped nanostructure. changed. In case the secondary or side reactions possess numerous
NTs can be produced with length to diameter (aspect) ratio of up to electrons it lowers the large molar mass and alters the polymer
132,000,000:1, considerably above any other material. They density, resulting in reduced performance of cement suspensions
possess atypical properties, which are precious for applications in [32,170]. For both chains to combine and paired simultaneously,
diverse felds of materials science and nanotechnology [32,123]. longer side groups and strong charge density from one to other
Particularly, due to their unusual thermal conductivity, mechanical reaction end must form. Usually, polycarboxylate is used in
and electrical characteristics CNTs can be used as additives for concrete as high range water reducer (HRWR). Inclusion of PCE
diverse structural applications. NTs are afliated to the fullerene allows in controlling the concrete workability better at lower water
family, in which the long and hollow construction with the walls to cement ratios.
created by one-atom-thick sheets of carbon so called grapheme The characteristics of PCE in concrete rely on its amount,
makes them diferent. Such sheets can be rolled at defnite where elevated amount may cause in false setting without any
orientations, where the revolving angle and radius together hydration incidence in the concrete [171]. Aside, addition of PCE
determines the attributes of CNTs [146]. Nanotubes are divided at required level can create Self Compacting Concrete (SCC)
into single-walled NT (SWNT) and multiwalled NT (MWNT). which enhances the workability of concrete. It also cxreates a fow
Individual NTs are aligned in the form of ‘‘ropes” that holds them concrete with enormous effects at small and elevated intensity
mutually by van der Waals forces or via pi-stacking [167,168]. region. Other beneft of PCE inclusion in UHPC or concrete is
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5.5. Titanium oxide layering or stacking fakes. Apparently, the kaolin particles are
identical to the nanokaolin, where the morphologies after the size
Titania or titanium oxide (TiO2) has widely been used as conversion from microparticles to nanoparticles ofer wider surface
pigment in foods colouring, paints, photocatalyses, implants, solar area. In the concrete, nanokaolin is treated to form extra reactive or
cells, and many other applications. Normally, it is resourced from stable product called nanometakaolin. Being a newly used
ilmenite, rutile and anatase phases and exists in nature as minerals’ supplementary ingredient in concrete, presence of nanometakaolin
phases such as rutile, anatase and brookite. At high pressure, TiO 2 improves the concrete properties unexpectedly [32]. The positive
is transformed to monoclinic baddeleyite and an orthorhombic efects of metakaolin in UHPC and other kinds of concretes are
structures, recently discovered at the Ries crater in Bavaria demonstrated [138]. Morsy et al. [185] showed that
[167,173]. Ilmenite and rutile form are the most abundant form of nanometakaolin inclusion in concrete could improve the mortars’
titanium dioxide-containing ore worldwide (98%). Heating above compressive strength by about 8–10%. Interestingly, the tensile and
temperatures 600° to 800 °C one achieves the metastable anatase fexural strength enhancement of mortar containing
and brookite phases [174]. nanometakaolin was discerned to be nearly 10–15% compared to
Incorporation of TiO2 into UHPC and other concretes revealed plain OPC [185,186]. Despite the advantages of nanometakaolin
remarkable infuence on self-cleaning capability and contributed as incorporation into mortars to improving the performance some
green material implementation in engineering construction [173]. shortcomings on the application of in UHPC were identifed.
Jubilee Church in Rome (Italy) exploited this self-cleaning Actually, lacking of raw kaolin in certain nations makes
attribute of TiO2 in buildings, materials’ paving and product nanometakaolin unpopular than celebrated silica fume. Thus,
fnishing [126]. TiO2 provides accelerated strength of concrete at standard guidelines and commercial protocols must be developed
early age, wherein the concretes performance and abrasion for large scale production of nanokaolin and nanometakaolin as
resistance both are enhanced [175]. TiO2 acting as glassy layer useful nanomaterial alternative to concrete for serving the
(extreme porosity) or pigment in the exterior of the particles in construction industries.
UHPC and concrete modifes their microstructure and thus the
performance. Moreover, such layers can react with the hydration 5.7. Nanoclay
gel products in mixing by producing protective layers, thereby
imparts self-cleaning capacity to the surface of concrete. This Nanoparticles of layered mineral silicates are called nanoclay.
selfcleaning action of titania in the exterior and coated concrete Based on these nanoparticles chemical compositions and
surface make them extremely durable with permeability. This morphologies, nanoclays are categorized into many classes
enhanced activity of titania incorporated concrete is regarded as including montmorillonite, bentonite, kaolinite, hectorite, and
fbre reinforced system that mimics the glassy fbre efect. It is halloysite. It is one of the most inexpensive materials with
realized that refnement and tailoring of the hydration gel via such benefcial outcomes in polymers. It is prepared from deposits of
fbres can be useful for the production of concrete with improved montmorillonite mineral having platelet structures of average
strength and prolonged durability [176]. Yet, health safety is a thickness of 1 nm thick and width of 70–150 nm. It possesses many
major concern related to the usage of TiO 2 because of its dusty good qualities and an outstanding base material for nanotechnology
nature where small dosage can result in notable environmental manoeuvring. These notable attributes are the stability, interlayer
impact especially to workers during packaging and manufacturing. spacing, elevated hydration and swelling capacity as well as strong
Some reports exhibited that TiO2 generates infammation and chemical reactivity. Clays and their improved organic products can
causes cancer to factory workers [175]. Consequently, it must be be analyzed via simple and modern instruments that can evaluate
handled with care, particularly during mixing and process of TiO2. the chemical compositions. These tools include gravimetric
analyser, inductively coupled plasma (ICP) or X-ray fuorescence
5.6. Nanokaolin (XRF) spectroscopy, cation exchange capacity (CEC) using
standard ammonium acetate technique, surface area determination,
Nanokaolin is a by-product of kaolin also called kaolinite, a Fourier transform infrared spectroscopy (FTIR), powdered X-ray
very important industrial clay mineral with the chemical formula of difraction (PXRD) and so on [58,88–90]. These clays are also
Al2Si2O5(OH)4 [177,178]. This is a silicate mineral with many distinguished via cation exchange capacity that can difer broadly
layers, where one tetrahedral layer is connected via oxygen atoms based on the source and nature of clay. The clay purity can
to another octahedral layer of alumina [179]. Kaolinite enriched infuence the nanocomposite behaviours. Therefore, it is signifcant
rocks are generally called kaolin or china clay [180]. This clay to obtain montmorillonite with minimal impurities such as
encloses white mineral that called dioctahedral phyllosilicate that is crystalline silica (quartz), amorphous silica, calcite and kaolin
formed by chemical changes of aluminium silicate minerals [187]. For the clays purifcation, several techniques have been
including feldspar [181]. For ceramic applications, kaolin is heat developed such as hydrocyclone, centrifugation, sedimentation
treated and altered into Al2O3.2SiO2·2H2O. After treatment or technique and chemical treatment [183].
endothermic dehydration crystalline phase of kaolin is transformed Clays are regarded as economical and easily accessible
to amorphous structures [182], where the new phase is known as materials. Despite their abundance worldwide, the guideline and
metakaolin. IT contains amorphous silica and alumina with some methods for transforming clay to nanomaterials is not well
hexagonal layering [183], which is very reactive pozzolan and documented yet. It is thus important to explore the constructional
reveals comparable reaction as silica fume. Furthermore, by
benefts and disadvantages of nanoclay as potential materials,
refning the microstructure of metakaolin both strength can although it has been diversely employed in the polymeric system.
durability can be improved, thereby allows consistent water Nonetheless, the proof on the improvement in the material
penetration. This properties make kaolin strong and cost efective hardness, thermal stability, barrier coating, and solvents together
than silica fume [32,184]. with the enhancement in the electronic and novel types of materials
Nanokaolin is generated following either top-down or bottom- are required. In the construction process, nanoclay is used as an
up approach, where the fnal product is infuence by the processing additive to improve the mechanical and binding concrete
conditions. Usually, the generation of nanokaolin comprised of
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characteristics. Morsy et al. [185] acknowledged that the nowadays, as nanomaterials become incorporated into concrete
enhancement in the compressive and tensile strength of mortar products in rising amounts it may help to develop an understanding
cement in the presence of nanoclay as additive. Furthermore, the of their interaction with the environment. Nanotechnology has the
thermal properties of concretes can be enhanced via the inclusion potential to dramatically change the strength, sustainability, and
of nanoclay as cement additive in the paste [188,189]. Qian et al. whole properties of concrete. Hamers [192] have
[150] studied the inclusion of nanoclay with water (worked as the
inner water provider to promote hydration alongside the
microcracks). It was shown that the recovery level could be
considerably improved with the incorporation of nanoclay in the
mixtures. The mechanism of healing depended on the reaction
between calcium hydroxide and nanoclay to formulate CSH gel led
to healing the crack.
5.8. Nanoiron
5.9. Nanosilver
Commonly, gaseous CO2 is released from OPC concrete during This research was supported and funded by the Universiti
the cement clinker's de-carbonation of lime and calcination Teknologi Malaysia Centre of Excellence (UTM COE) research
reactions. Using nanomaterials based self-healing technology grant Q.J130000.2409.04G00 and Fundamental Research Grant
emission of CO2 can remarkably be reduced. Currently, world's Scheme (FRGS) grant R.J130000.7822.4F722. The authors would
development exclusive of concrete is beyond imagination [193]. like to thanks the grants provider, namely Universiti Teknologi
History tells us that without concrete the wonderful structures like Malaysia and Ministry of Higher Education, staf from Material
Sydney Opera House, the Chrysler Building, or Taj Mahal could and Structure Laboratory, School of Civil Engineering, Universiti
not have existed. Furthermore, the skyscrapers in metropolis all Teknologi Malaysia, and the EM Malaysia Sdn. Bhd. and EMRO
over the world would have reached to such striking altitudes Japan for their support and cooperation in conducting this research.
without the usage of celebrated concretes. In every aspect,
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