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Geopolymer concrete with metakaolin for sustainability: a comprehensive

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Article in Environmental Science and Pollution Research · January 2022

DOI: 10.1007/s11356-021-17849-w

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Environmental Science and Pollution Research
https://doi.org/10.1007/s11356-021-17849-w

ENVIRONMENTAL SUSTAINABILITY AND REMEDIATION

Geopolymer concrete with metakaolin for sustainability:

a comprehensive review on raw material’s properties, synthesis,
performance, and potential application
Bharat Bhushan Jindal1 · Thamer Alomayri2 · Assaedi Hasan2 · Cyriaque Rodrigue Kaze3

Received: 1 October 2021 / Accepted: 25 November 2021

© The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature 2021

Abstract
In the last three decades, the gigantic demand for sustainable and environmentally friendly concrete with reduced environ-
mental footprints has resulted in the development of low carbon concretes such as geopolymer concrete. Metakaolin which
is commonly used as an admixture or partial replacement of cement owing to its most effective pozzolanic properties, which
improve the microstructure and strengthen the mechanical and durability properties of cement concrete, has been investigated
as a precursor in geopolymer concrete. Several studies have been conducted to comprehend the effect of metakaolin as an
additive in geopolymer mortar and concrete prepared with various aluminosilicate sources as precursors such as fly ash and
rice husk ash to enhance geopolymerization, densify microstructure, and elevate durability. The present paper recapitulates
these investigations primarily concentrating on the various properties of metakaolin-based concrete. The effect of various
factors such as alkali content, solids/liquids ratio, alkali reactant ratio, molar ratio, water content, and curing regime has
been compiled. Most of them revealed that metakaolin is used as a precursor and yields better geopolymer products. XRD
studies reported the peaks demonstrating the development of enhancement in hydration products in comparison to other
precursors. Examination of SEM graphs reveals that the addition of a smaller quantity of silica-rich materials densifies the
microstructure of geopolymers and produces higher mechanical strength. Durability studies reveal that metakaolin geo-
polymers possess better water resistance, thermal resistance, and anti-corrosion properties. The possible applications of
metakaolin-based geopolymeric materials are also pointed out. The comprehensive knowledge presented here is expected
to support the prospective researchers to decide their future course of the research area.

Keywords Geopolymer · Metakaolin · Sustainability

Introduction of construction materials at a gigantic scale. Since OPC

The increase in worldwide population, projected as more
than 9.8 billion in 2050, demands sustainable construc-
tion, urbanization, industrialization, and infrastructure.
It intensifies the need for the ever-growing requirement
Responsible Editor: Philippe Garrigues
* Bharat Bhushan Jindal
bharat.jindal@smvdu.ac.in
1
School of Civil Engineering, Shri Mata Vaishno Devi
University, Katra, Jammu and Kashmir, India
2
Department of Physics, Umm-Al-Qura University,
Makkah 21955, Saudi Arabia
3
Department of Inorganic Chemistry, Faculty of Science,
University of Yaounde-I, Yaounde, Cameroon
concrete is a broadly accepted construction material, so,
the worldwide production of concrete has surpassed other
types of building materials over the past 50 years, with
the rate of growth in per capita consumption exceeding
rates of population growth (United Nations 2017). Port-
land cement manufacturing process alone releases up to
5–8% of current anthropogenic carbon dioxide worldwide
(Chen et al. 2010; Gartner 2004; Meyer 2009). A huge
amount of ­CO2 is released during the calcination of lime-
stone, and the combustion of the fossil fuels is nearly 1
ton for each 1 ton of cement production (Davidovits 1993;
Huntzinger and Eatmon 2009; Li et al. 2011; Peng et al.
2013). However, some of the studies have shown that up to
25% of the ­CO2 emission during the cement manufactur-
ing process can be reabsorbed if recycling practices are
adopted where concrete obtained from demolition waste

13
Vol.:(0123456789)

of concrete structures when exposed to carbonation during
post-use phases (Brandt et al. 2009; García-Segura et al.
2014; Kajaste and Hurme 2016; Latawiec et al. 2018).
During the last few decades, research is focused on devel-
oping alternative cementitious materials to reduce the
release of greenhouse gases, which can help in the devel-
opment of a sustainable environment.
The ardent need for sustainability propelled the
researcher to investigate the alkali-activated binders,
which are also termed as “geopolymers” and can be pre-
pared from the aluminosilicate-rich materials by the geo-
polymerization process. The research in this field also got
encouraged as industrial waste by-products such as fly ash,
rice husk ash, ground-granulated blast furnace slag, and
red mud are produced in huge amounts and are found to be
very rich sources of aluminosilicates that can be utilized
in the production of geopolymer-based binders. Any poz-
zolanic material containing silica and alumina and is easily
soluble in alkaline solutions can be utilized as a precur-
sor for the geopolymerization process in geopolymers (Ye
et al. 2014). Geopolymerization is simply defined as the
reaction which liberates silica, alumina, and lime, while
aluminosilicate source material interacts with an alkaline
activator to form aluminate-silicate hydrate and finally
condensation and hardening (Van Jaarsveld et al. 1997;
Khale and Chaudhary 2007). The silica content plays a
leading role in geopolymerization, which produces geo-
polymeric gel responsible for the development of mechani-
cal properties (Palomo et al. 1999a, b).
Geopolymers due to their comparatively higher mechan-
ical strength and excellent stability in high temperature
(Aydin et al. 2012; Jindal, et al. 2017a, b, c, d), better per-
formance in adverse environmental conditions (Abdulka-
reem et al. 2014; Bakharev 2005; Hussin et al. 2014), low
creep and shrinkage (Wallah 2010; Sagoe-Crentsil et al.
2013), and better durability (Jindal, et al. 2017a, b, c, d;
Law et al. 2014) to ordinary Portland cement along with the
emission of lesser carbon dioxide during the manufacturing
process has fascinated the researchers worldwide (Cheng
et al. 2015c; McLellan et al. 2011; Yang et al. 2016; Yang
et al. 2013; Ye et al. 2014). Available literature reveals that
various industrial waste products such as fly ash, GGBFS,
RHA, and metakaolin (MK) have been used as a source of
alumina and silica for the preparation of geopolymers. MK
which can be obtained from the calcination of kaolin clay
and is rich in silica and alumina has also been used as a base
material and in combination with other waste materials in
the preparation of geopolymers.
This review paper presents an extensive review of avail-
able research from various sources on the use of metakaolin
in the formulation of geopolymer systems and its effect on
their mechanical and durability properties along with further
exploring the possibilities of industrial applications.
13
Environmental Science and Pollution Research
Materials
Metakaolin (MK)
Metakaolin is a product or by-product manufactured from
China clay (kaolin) on heating it at a higher temperature, a
very effective pozzolanic material used in concrete. In the
1960s, metakaolin was successfully incorporated into the con-
crete used in the construction of several large dams in Brazil.
Metakaolin is used as a replacement to OPC for improving
various properties of cement concrete.
Manufacturing process and structure of metakaolin
Metakaolin is one type of anhydrous aluminosilicate mate-
rial. It can be produced by calcination or dihydroxylation of a
naturally available clay mineral kaolinite ­[Al2Si2O5(OH)4] at
500–900 °C, as shown in Fig. 1. In kaolinite (China clay), the
hydroxyl ions strongly bonded to the aluminosilicate frame-
work structure, which can only be eliminated at temperatures
above 550 °C (Fernández-Jiménez et al. 2008). Kaolinite when
subjected to a higher temperature, the dihydroxylation of it
takes place and it losses the available water molecules termed
structural water. The removal of structural water results in
the formation of a highly disordered molecular structure (see
Fig. 2) and the product so formed is termed metakaolin. The
nature of the materials so obtained, i.e., metakaolin is highly
amorphous in contrary to kaolinite which is a crystalline
material (Bheel et al. 2021; Kakali et al. 2001; Sperinck et al.
2011). This amorphous nature of the metakaolin is considered
to be very reactive when exposed to an alkali/alkaline solution
(Fernández-Jiménez et al. 2008; Granizo et al. 2000; Kakali
et al. 2001). Moreover, the rich content of silica and alumina
in metakaolin makes it a very good mineral admixture and can
be used in conventional cement concrete for improvizing the
mechanical and durability properties (Kou et al. 2011). The
improvement in mechanical properties and durability of con-
crete with MK are due to the highly reactive pozzolanic nature
which it reacts with calcium hydroxide (Ca(OH)2) and forms
hydrated calcium aluminates and silicon aluminates along with
its filling effects (Nuaklong et al. 2018).
Metakaolin, unlike other supplementary cementitious mate-
rials (SCMs), is not an industrial by-product. It is derived from
naturally occurring minerals and is manufactured under care-
fully controlled conditions to refine its physical properties such
as color, particle size with a high degree of purity, and poz-
zolanic reactivity.
Chemical composition and physical properties of MK
Chemistry of metakaolin and chemical composition The
chemical compositions of some metakaolin powders
Environmental Science and Pollution Research
Fig. 1  Flow chart depicting
the manufacturing process of
metakaolin
obtained from different calcined kaolins between 550 and
750 °C used as solid precursors for the geopolymer synthesis
are reported in Table 1. This table presents the data of pub-
lished works focussed on metakaolin originating from dif-
ferent continents around the world namely Africa (Balo et al.
2018; Tchakouté et al. 2017; Tchinda Mabah et al. 2019),
Europe (Hasnaoui et al. 2019; Moutinho et al. 2019; Pouhet
et al. 2019; Rovnaník et al. 2018), Asia (Duan et al. 2015; Lv
et al. 2019; Wan et al. 2019; Zhang et al. 2009), and America
(Arellano-Aguilar et al. 2014; Istuque et al. 2019) used as
raw material/precursor for the preparation of geopolymer
products. Additionally, the sum of major oxides (Si and Al
oxides) in different samples is less than 70 wt.% justifying
their use as good aluminosilicate solid precursors for geo-
polymer synthesis. However, the presence of other oxides
excluding alkali oxides (Ca, Na, Mg) behaves as fillers or
micro aggregates during the geopolymerization reaction due
to their non-integration into the geopolymer network. There-
fore, these oxides, in certain proportions, become deleterious
Fig. 2  Metakaolin formation by
the dihydroxylation of kaolinite
(Sperinck et al. 2011)
for the strength development of geopolymer materials due
to their non-participation in the reaction medium, indicating
their non-dissolution.
Mineralogy of metakaolin Metakaolin is an amorphous
material obtained from calcined kaolin between 550 and
750 °C (Elimbi et al. 2011; Kaze et al. 2017). The dihydrox-
ylation of the kaolinite mineral phase contained in kaolin
clay after calcination produces metakaolin. From numerous
published works, metakaolin appears as one of the most alu-
minosilicates widely studied.
Physical parameters After the conversion of kaolin to
metakaolin, this latter becomes finer compared to the first
one. These fine particles justified their reactivity in contact
with the alkaline solution. The mean particle size, specific
surface area, and bulk density of metakaolin found in the
literature are reported in Table 2.
13
 Environmental Science and Pollution Research

Alkaline activators

(Istuque

2019)

58.39
35.47
et al.

2.71

1.44
0.01

1.51
0.30

0.10
The presence of highly alkaline activators is required for

/
/
the geopolymerization reaction to take place. Alkaline
et al. 2014)
(Arellano-
activators enable the dissolution of reactive amorphous
Aguilar

aluminosilicates for the polycondensation of oligomers

75.41
22.91
0.64

0.52
0.52

0.42
and form a compact microstructure. Hence, the chemical

/
/
/

/
/
and physical properties of alkaline solution play an impor-
tant role in consolidated or activated materials behavior.
(Lv et al.
America

2019)

51.90
45.99

The main alkaline activators used in geopolymers synthe-

0.23

0.03
0.12

0.47
0.05
0.26

0.27

0.77
sis are hydroxides and alkali salts, and the most commonly

/
/
used are NaOH, KOH, ­Na2CO3, ­Na2SO4, and ­Na2SO3.
(Duan

2015)

55.57
41.55
et al.

0.56

0.43

0.97
Sodium or potassium hydroxides
/
/

/
/

/
/
(Wan et al.

NaOH and KOH are the most commonly used alkali solutions
2019)

52.80
43.70

for geopolymers synthesis in previous works. Both metal ions

0.60

0.50
1.20
0.20

from these solutions affect the geopolymerization reaction and

/
/

/
/

/
microstructural and structural properties differently. In the
(Zhang

2009)

52.92
43.85

­ a+ ions from NaOH are used and improve

point of size view, N
et al.
Asia

0.59

0.18
0.28

0.99
0.18

0.17
0.17

0.49

0.83

the dissolution rate and help in the better stabilization of the

/

silicate monomers and dimers in the solution compared to

(Pouhet

larger ­K+, which further improves the rate of condensation and

2019)

68.10
24.10
3.73

0.08
0.91

1.14
0.35

0.03
0.22
et al.
Table 1  Chemical compositions of some metakaolin powders taken in various studies across various countries

accelerates the reaction kinetics (Toniolo et al. 2018). By the

way, potassium cations in literature are known as a facilitator
(Tchakouté (Rovnaník (Moutinho (Hasnaoui

of the formation of larger silicate oligomers resulting in the

2019)
et al. 2020) et al. 2018) et al. 2019) et al.

55.0
39.0
1.80
0.60

1.50

1.23

best setting, compact structure, and high compressive strength

/

/
/

/
/

(Xu and Van Deventer 2000). Although the fact is that using
KOH allows obtaining geopolymer products with good
characteristics, and NaOH due to its low-cost production is
51.94
39.83
2.09

0.09
0.13

1.66
1.21
0.07
0.31

2.43

used extensively as a hardener in previous works (Cyr et al.

/
/

2012; Wang et al. 2005).

Europe

58.70
38.50
0.70

0.04

0.85
0.20

0.49

0.02
0.38

1.67

Sodium or potassium hydroxides mix Na or K silicate

/
/

The combined mixture of NaOH/KOH with Na/K silicate

gives the most interesting performances compared when
48.31
40.48
2.62

0.15

1.30
0.04

4.45

0.02

0.02
0.36

0.03

1.42

alkali sources are used alone. For more reactivity, the

mixture requires at least 24 h of cooling at room temperature
et al. 2019)

before use and to allow depolymerization of long silicate

(Tchinda
Mabah

chains into monomer, dimer, and tetramer that improves

47.10
33.90
0.99

0.42
0.21

0.83

0.03
0.20

0.79

their reactivity by avoiding hot system resulting in friendly

/

/
/

use and synthesis. However, the molar ratios of ­SiO2/

(Tchakouté (Balo et al.

Na2O and ­H2O/Na2O in preparing the alkaline hardener are

et al. 2017) 2018)

41.46
31.47
7.65

0.62
0.15

1.50
0.51
0.09

0.00
0.65

0.06

1.20

determinants for the geopolymer. These ratios appear among

the key parameters that govern the resulting characteristics of
synthesized products. Published papers dealing with different
aluminosilicates (fly ashes, metakaolin, volcanic ashes, and
Africa

1.25

0.00
0.03

1.97
1.23
0.14

0.00
0.06

0.01

0.73
62.0
30.8

laterites), indicate the use of ­SiO2/Na2O and ­H2O/Na2O ratios,

ranging between 1–2 and 10–20, respectively, to synthesize
geopolymer with desired properties (Assaedi et al. 2020;
Oxides

Kaze, et al. 2018a, b; Kaze, et al. 2018a, b; Luukkonen et al.

(wt.%)

Al2O3
Fe2O3

Na2O
MgO

MnO
P2O5
TiO2

L.o.I
SiO2

CaO

K2O

SO3

2017; Ravikumar and Neithalath 2012; Shi et al. 2018). By

13
Environmental Science and Pollution Research
Table 2  Physical parameters Type of study
of metakaolin obtained from
calcined kaolin at 700 °C
Kenne et al. (2015)
Živica et al. (2012); Balo et al. (2018)
Hawa et al. (2013a, b)
Celerier et al. (2018)
Aupoil et al. 2018 (Aupoil et al. 2019)
the way, the chemical and mineralogical compositions of solid
precursors should be well known before, and the interval of
ratios abovementioned could be used for the synthesis.
Knowing that the geopolymer products consolidated with
sodium silicate give high characteristics, their production
strongly required more energy and high temperature. Sodium
silicate can be obtained by heating a mixture of sodium
carbonate and silica sand at 1400 °C. To overcome this
required energy, some silica sources from biomass were
used to prepare glass silicate as the alternative solution by
researchers (Kamseu et al. 2017; Tchakouté et al. 2016)
Various studies conducted so far on the alkaline activation of
materials have shown that alkali silicate solutions with a low
­SiO2/Na2O ratio are the most effective activators and more
efficient for obtaining geopolymers with better mechanical
performance. It is only possible by adding NaOH to the
commercial solution to increase the pH of the solution and
make more reactive the silicate species that play a vital role in
the formation of geopolymeric gel. Like any basic compound
and because of its corrosive character, the handling of the
sodium silicate solution must be with precautions.
Geopolymerization of metakaolin
The geopolymerization reaction of metakaolin was exten-
sively monitored by many authors using different experi-
mental techniques. Elimbi et al. 2011 (Elimbi et al. 2011),
in their study, reported the effects of temperature during
the calcination of kaolinite clays on the microstructure and
mechanical properties of metakaolin cement. They found
that the setting time using the Vicat needle decreased from
130 to 40 min as well as increased the compressive strength
from 11.9 to 36.4 MPa. The decreasing trend of the proper-
ties is related to the rise of the amorphous or reactive phase
that occurred during calcination. The increased amorphous
phase favored a higher degree of geopolymerization result-
ing in high polycondensation. Zhang et al. 2012 (Zhang et al.
2012) used isothermal conduction calorimetry (ICC) and
studied the kinetics of geopolymerization of sodium silicate-
activated metakaolin by varying the reaction temperature
from 20 to 40 °C. They found that on varying the silica
modulus from 1.60 to 1.20, the fractional reaction extent
Specific surface area Particles size Specific density
distribution d50
128 ­cm2/g 15 µm 2.54–2.56 (g/cm3)
38.7 ­m2/g 772 nm 2.582 (g/cm3)
19.9 ­m2/g 9.7 µm 2.65 (g/cm3)
16.32 ­m2/g 6.31 µm
17.0 ­m2/g 10.0 µm
18.0 ­m2/g 10.3 µm
increased from 0.12 to 0.26 after 72 h at 20 °C. However,
on escalating the reaction temperature from 20 to 40 °C,
reaction extent improved from 0.24 to 0.35 when the alka-
line solution was of silica having the modulus of 1.2. They
concluded that at a temperature of 40 °C, the rapid polymeri-
zation/polycondensation of oligomer species occurs. Based
on the work described above, typically found that geopoly-
merization get influenced the mineralogy or raw material,
reaction temperature, and an alkaline solution. With the use
of metakaolin (mainly composed of reactive silica and alu-
mina) as a solid precursor, the geopolymerization reaction
is elaborated as follows:
(i) The dissolution step involves the breaking down of
Si–O-Si and Si–O-Al bonds of the minerals to form
reactive precursors (Si(OH)4 and Al(OH)4) in the
solution.
(ii) The restructuring stage intervenes in the solution,
when the reactive aluminosilicate precursors are
mobile and thermodynamically stable, before being
gelled.
(iii) The polycondensation step consists of the polym-
erization of the oligo-sialate molecules followed by
their reticulation and network formation of polysi-
alate with the 3 D framework.
These steps are summarized in a representative schematic
in Fig. 3 proposed by Yao et al. 2009 (Yao et al. 2009).
Properties of metakaolin‑based geopolymer
mortar/concrete
In the current section, various properties of the metakaolin-
incorporated geopolymer mortar and concrete are illustrated
as per the studies available so far.
Bulk density
The bulk density of geopolymer concrete is significantly
influenced by several parameters, such as curing type
(Rovnaník 2010), type of geopolymer precursors (Sarath
Chandra Kumar and Ramesh 2016), nature of alkali silicates
13
 Environmental Science and Pollution Research

Fig. 3  Sketch of the geopolymerization process of metakaolin by ▸

alkaline solution activation (Yao et al. 2009)

(Lizcano, et al. 2012a, b), and the molar concentration

of metal hydroxides. The sodium-based (Na-type)
geopolymer shows a lower density than potassium-based
(K-type). K-based geopolymers show less porous and
better homogeneous structures than Na-based geopolymers
(Lizcano, et al. 2012a, b). On the other hand, metakaolin
geopolymers are less dense than ordinary Portland cement,
fly ash, and GGBFS-based geopolymers. It is reported that
their density range is between 1.20 and 1.80 g/cm3 (Liew
et al. 2016). Therefore, the metakaolin-based geopolymer
concrete is a lightweight product, having the bulk density in
the range of 2.10 to 2.40 g/cm3 in comparison to the range
of 2.25 to 2.40 g/cm3 of fly ash-based geopolymer concrete
(Marín-López et al. 2009; Vijai et al. 2010).
The bulk density of hardened geopolymer concrete
decreases with rising curing temperature because GP
structure becomes less dense, and hence lesser compact-
ness (Rovnaník 2010). Curing at a temperature (below
60 °C) speeds up the hardening process and improves the
physical properties of the geopolymer concrete. On the
contrary, the rapid setting of slurry at high temperatures
(80–100 °C) restrains its transformation into a compact
and robust structure, which negatively affects the physical
properties (Mo et al. 2014).

Workability

Geopolymers do not show the hydration reaction due to

which the water requirement during mix design is lesser
as compared to conventional concrete. The lesser water
available in the geopolymer mix reduces the workability
(Chindaprasirt et al. 2007; B.B. Jindal, et al. 2017a, b, c,
d; Reddy et al. 2010; Srinivasreddy et al. 2013; Yang and
Song 2009). Workability varies with various factors such
as alkali concentration, binder content, type of binder, and
ambient temperature during the preparation of the mixture.
It may, however, get improved by adopting the methodol-
ogy of premixing the alkaline solution, superplasticizer, and
extra water and then mixing to the dry ingredients of the mix
(Nuruddin et al. 2011).
The effect of superplasticizers on alkali-activated mor-
tars is quite different from its effect on cement mortars. The
superplasticizer used in alkali-activated mortars increases
the workability but may adversely affect the development
of the compressive strength (Chindaprasirt et al. 2007).
Naphthalene-based superplasticizers improve the workabil-
ity of geopolymers (Jindal, et al. 2017a, b, c, d; Palacios and
Puertas 2005; Rangan 2009). A superplasticizer content of
up to 2 wt.% can enhance the workability without affecting
the compressive strength of geopolymer (Jindal, et al. 2017a,

13
Environmental Science and Pollution Research
b, c, d; Rangan 2009). The workability of a geopolymer also
varies with the quantity of alkali content. On increasing the
alkali concentration, the workability decreases.
Mineral admixtures are generally in use to improve the
mechanical and durability properties of concrete. Metakao-
lin, when used as an admixture in conventional concrete,
results in decreased workability. Studies reported the
decrease in workability with metakaolin is due to its higher
water demand because of its higher fineness and plate-like
structure (Güneyisi et al. 2012; Melo and Carneiro 2010;
San Nicolas et al. 2013; Weng et al. 2013). Superplasticizer
with an addition of an admixture containing CaO has pro-
vided enhanced workability without any adverse effect on
compressive strength (Deb et al. 2014; Jindal, et al. 2017a,
b, c, d; Pacheco-Torgal et al. 2011). However, Alanazi
et al. (2017) reported enhanced workability of the metaka-
olin-based geopolymer concrete on partial replacement of
metakaolin with slag.
Setting time
In general, the setting time is influenced by several param-
eters such as the composition of the alkaline solution, the
ratio of alkaline liquid to binder content by mass, curing
type, and curing temperature of geopolymers. In our ear-
lier studies, the use of the various type of mineral admix-
tures to enhance the properties of geopolymers products
is well elaborated (Rovnaník 2010; Sperinck et al. 2011).
Rovnanik (2010) reported that the geopolymer mixture
at ambient temperature shows a hardening process within
the first 24 h, whereas if cured at low temperature, it took
even 7 days. It is observed that for air-cooled specimens,
the setting time is 4 days, whereas in the case of the heat
curing method, the specimens were set within 2–4 h.
Nano-silica is found to be very effective to acceler-
ate the setting process in cement as well as geopolymer
concrete due to its finer particle size and enhanced sur-
face area, which reduces the dormant period, enhances
the hydration, and accelerates the geopolymerization
(Rovnaník 2010; Sarath Chandra Kumar and Ramesh
2016; Sperinck et al. 2011). Gao et al. (2013) reported
a decrease in the setting times of geopolymers with the
addition of nano-SiO2 (NS), which attributes to its high
nanoparticle activity and promotes the geopolymeriza-
tion reaction rate. The setting time further declined with
an increase in the solids-to-liquids ratio. The specimen
with 1% NS showed better compactness. Gao et al. (2014)
reported an increase in the setting time of nano-SiO2
admixed metakaolin geopolymer increased ­S iO 2/Na 2O
ratio because increased sodium silicate content results in
a more viscous liquid.
De Silva et al. (Silva, Sagoe-Crenstil, and Sirivivat-
nanon 2007) observed that alumina content significantly
controls the setting of geopolymers. The setting process
deaccelerated with an increased S ­ iO2/Al2O3 ratio of the
initial mixture. An optimal ­SiO2/Al2O3 ratio in the range
from 3.5 to 5.5 gives higher compressive strength, which
also depends on activator type and curing conditions. Set-
ting time can be decreased by increasing the Al content,
but it will also decrease the strength due to a decrease in
­SiO2 content. Pangdaeng et al. (2015) described that the
presence of calcium-containing materials in geopolymers
accelerates the setting process. Calcium provides addi-
tional nucleation sites for the precipitation of dissolved
species and results in faster setting and hardening.
The curing temperature plays a more significant role
in the geopolymerization process of geopolymers. In
general, as the curing temperature increases, the setting
time of geopolymer concrete decreases (Givi et al. 2010;
Liew et al. 2016; Marín-López et al. 2009). According
to Basil and Tareq (Al-Shether et al. 2016a), the type of
curing method significantly affects the setting of metaka-
olin-based geopolymer concrete. They said the optimum
temperature for curing is in the range of 32–48 °C under
sunlight or room temperature. Sunlight curing in the sum-
mer is effective and cheap when the ambient temperature is
higher than 35 °C. Halogen curing system for temperature
(50–55 °C) and hot-air electric oven (> 50 °C) is found
appropriate in cold weather.
Compressive strength
Lopez et al. (2009) reported that the strength gained by
metakaolin geopolymer concrete is higher than cement con-
crete. The higher strength achievement is due to the reason
that the calcined binder materials show a higher binding
strength. The development of the compressive strength of
GPC is observed to be significantly influenced by water con-
tent as well as the available Si/Al ratio in the mixture. The
compressive strength range in various studies is found to be
in the ranges of 20–100 MPa (Davidovits 1991; Lizcano,
et al. 2012a, b; Marín-López et al. 2009; Rangan 2008; Ste-
venson and Sagoe-Crentsil 2005). Arellano-Aguilar et al.
(2014) confirmed that even the metakaolin geopolymer with
a relatively low grade (50% MK–50% quartz) achieves com-
pressive strengths above 85 MPa after 28 days. The amount
of compressive strength gained by geopolymer indicates
the extent of the geopolymerization process. The higher is
the dissolution of source materials, producing more geo-
polymeric materials, and the higher will be the compressive
strength. The inclusion of slag can significantly improve the
compressive strength of metakaolin-based geopolymer con-
crete. Furlani et al. (2018) reported the effect of unprocessed
steel slag on the properties of the metakaolin geopolymer.
The authors reported the increase in the workability of geo-
polymer slurry on replacing metakaolin with slag. However,
13

they obtained the highest compressive strength of the mix
containing 40 wt% steel slag and 60 wt% metakaolin. On
contrary, the higher steel slag content showed detrimental on
the compressive strength. The authors further reported that
the calcium and magnesium oxides in the slag result in the
formation of stronger mechanical bonds. The compressive
strength gets influenced by the amount of geopolymeric-
gel, type of reaction products, the rate of calcination, tem-
perature, curing time, and relative humidity (García-Mejía
et al. 2016). Diffo et al. (2015) reported that the compressive
strength is also influenced by the rate of calcination of kao-
lin. Therefore, it is observed that for the development of high
compressive strength, the rate of calcination must be lower.
Ekaputri and Junaedi ( 2017) reported that the tempera-
ture of curing affects the compressive strength. They also
investigated the effect of polyvinyl alcohol fibers on the set-
ting, workability, and mechanical strength. The authors con-
cluded that curing at a temperature of 80 °C with 1% PVA s
significantly, the rate of geopolymerization is only affected
by the curing temperature and not by the inclusion of fibers.
Lo et al. (2017) reported that the addition of a small
quantity of nano-silica enhances the compressive strength
of MK geopolymer. The inclusion of 0.5% nano-silica
increases the compressive strength of the specimen from
58.3 to 71.1 MPa. In a recent study, Zawrah et al. (2020)
used nano-sand in the investigation of the properties of MK
geopolymer. Nano sand, which is white and contains 98.8%
­SiO2 with varying percentages (2.5, 5.0, and 7.5%), was
added to the MK geopolymer. The optimum dose of nano-
sand of 2.5% produced the specimen with a maximum com-
pressive strength up to 60.8 MPa, which decreased with the
increase of nano-sand content. Nano sand addition produces
additional geopolymeric gel, which improves the mechanical
strength up to the optimum level. On the contrary, higher
nano-sand adversely affects the compressive strength.
Liang et al. (2019) reported a study of the metakaolin
geopolymer with rice husk ash (RHA). Metakaolin geopoly-
mer paste is prepared by replacing the metakaolin up to 40%
with RHA. The geopolymer paste containing 70% metakao-
lin with 30% rice husk ash achieved the highest compressive
strength, which is 57.18% higher than the mix without rice
husk ash. The rich silica content in RHA significantly con-
tributed to the development of compressive strength.
Shrinkage cracking
Geopolymers show excellent thermal stability with low
shrinkage and are suitable for thermal applications up to
1100 °C (Davidovits 2002; Kamseu et al. 2010; Schmücker
and MacKenzie 2005; Trindade et al. 2017). Geopolymers
prepared with an alkaline solution containing potassium is
found to be better than sodium and can have better applica-
tion as a ceramic material to be used at high-temperature
13
Environmental Science and Pollution Research
exposure (Barbosa and MacKenzie 2003a; Davidovits 1989).
According to Subaer and Riessen (2007), the MK-based
geopolymer showed 2% shrinkage at a temperature up to
250 °C. However, better dimensional stability is between
250 and 800 °C. It is also observed that aggregate (quartz or
granite) helps in reducing the shrinkage to 1% (Subaer and
Van Riessen 2007). Geopolymer with 50% metakaolin and
50% fly ash provides better resistance to exposure to high
temperatures (Zhang et al. 2014).
The substitution of metakaolin by low-cost inert fillers
such as sand reduces the shrinkage cracking. Kuenzel et al.
(2014) found that the geopolymer mortars with sand > 10%
by volume percentage resisted heating to 110 °C without
cracking. The linear shrinkage value is observed to be lim-
ited by the sand particle because of the formation of a sup-
portive network with a fixed void volume. In another study,
authors (Kuenzel et al. 2013) pointed out based on dilato-
metry results that the use of sand as a filler diminishes the
initial shrinkage which is related to loss of free water from
8 to 1.5%. Moreover, the results show the shrinkage value is
independent of the filler size.
Acid resistances
Metakaolin-based geopolymer shows good stability in
aggressive liquids. Palomo et al. (1999a, b) reported a long
way back, that alkali-activated metakaolin samples showed
excellent stability on immersion in different types of acidic
solutions. The specimens immersed in acidic solutions such
as de-ionized water, sodium sulfate solution, ASTM seawa-
ter, and H
­ 2SO4 solution (0.001 M) showed excellent stability
up to 270 days. No deterioration in mechanical properties
was found when submerged in aggressive liquids. Geopoly-
mers immersed in an acidic medium show the transition of
the amorphous phase of the aluminosilicate network struc-
ture into a more crystalline one (Liew et al. 2016; Palomo,
et al. 1999a, b). Slaty et al. (2015) reported no decline in
mechanical properties when the specimen was in seawater
(having a pH value of 8). Also, a similar type of pattern was
noticed in sodium sulfate solution (5% ­Na2SO4) for up to
nearly 1 year.
Alternatively, geopolymers get showed severe deterio-
ration when put in HCl solution for an extended period,
which increases as the pH of the acid decreases below 6.5.
The highly acidic solution results in the dealumination of
the aluminosilicate. The acid attack breaks the Si–O–Al
bonds, which in turn raises the number of silicic acid ions
in the solution, ultimately leading to a loss of mass of the
polymeric structure. The authors further reported that the
addition of sand as a filler improved the durability of the
MK-geopolymer under ambient, de-ionized water, sodium
sulfate, and seawater conditions. However, the loss of mass
Environmental Science and Pollution Research
and the decline of the mechanical strength were observed in
a strongly acidic solution.
Recently, Aygörmez et al. (2020) found that exposure to
hydrochloric acid depolymerized the geopolymeric prod-
ucts, which caused the loss of strength. However, the less
degradation of geopolymer products under the influence of
acid in comparison to Portland cement is due to the strong
alumina-silicate bonds. In acidic exposure, more crystalline
phases form, which increases the stability of geopolymers.
Freeze–thaw
Freezing and thawing cycles cause damage to the concrete
structures that are located in cold areas and weaken their
long-term performance. Therefore, to check the durability
of a structure, its free-thaw resistance needs to be evaluated.
The concrete structure, when subjected to temperature
fluctuating above and below freezing, then the region
continuously sucks water from the adjacent region and
results in repeated loss of concrete mass and deterioration of
its mechanical properties (Fu et al. 2011; Zhao et al. 2019).
According to ACI, the freeze–thaw effect on the durability
of concrete is defined as the percent ratio of the final value
of dynamic modulus of elasticity after several freezes and
thaw cycles to the initial value before the freeze–thaw
cycles (Alanazi et al. 2017; Hamoush et al. 2011). A limited
number of reports describe the freeze–thaw effect on the
metakaolin geopolymer (MKG).
Alanazi et al. (2017) performed 30 freeze–thaw cycles
on metakaolin geopolymer concrete. The authors reported
that MKG, the frost resistance of the geopolymer, decreases
with increasing the water content. The addition of slag
decreased the percentage of mass loss. Also, freeze–thaw
cycles substantially affect the durability of geopolymer con-
crete by spalling the concrete surface which leads to the loss
in weight. Therefore, it can be concluded that the percent-
age of water in the mix significantly affects the freeze–thaw
resistance of geopolymer.
Bond strength
Geopolymer concrete is found to have better bond strength
in comparison to OPC concrete. Sarkar (2010) reported that
during the pull-out test on geopolymer concrete and OPC
concrete, higher bond strength was noticed in geopolymer
concrete than conventional concrete. Geopolymers form
a stronger bond with the aggregates due to their inherited
alkaline solution (Boopalan and Rajamane 2017; Doguparti
2015; Hu et al. 2008; Kathirvel et al. 2017; Sofi et al. 2007).
The bond strength of geopolymer concrete is closely associ-
ated with its tensile and compressive strengths (Chang et al.
2009; Topark-Ngarm et al. 2015). Geopolymer prepared
from high-calcium fly ash is more suitable as it develops a
significantly higher compressive strength and better bond
strength (Topark-Ngarm et al. 2015).
Metakaolin-based geopolymer mortars show superior
bond strength in comparison to cement mortars (Alanazi
et al. 2016). The bond strength can further be enhanced by
incorporating a suitable admixture into metakaolin geopoly-
mer mortar (Hawa, et al. 2013a, b; Khater 2013). Khater
et al. (2013) reported that pozzolanic activity of silica fume
enhances the properties such as compressive strength,
abrasion resistance, and bond strength when silica fume
is admixed in metakaolin-based geopolymer by producing
additional C-S–H gel.
Factors affecting properties of metakaolin
geopolymer concrete
The properties of geopolymer mortar and concrete are influ-
enced by various parameters such as alkali concentration,
initial solids/liquid ratios, alkali reactants ratios, molar ratios
of Si, Al, Na, and ­H2O contents, water content as well as
curing regimes.
Alkali concentration
NaOH concentration significantly influences the mechani-
cal properties and the content of the amorphous phase of
metakaolin-based geopolymers. Alkali solution speeds up
the solubility and dissolution of metakaolinite particulates
resulting in accelerating the geopolymerization which fur-
ther enhances flexural strength, compressive strength, and
apparent density of the geopolymer with an increase of
NaOH concentration within 4–12 mol/L (Kamarudin et al.
2011; Wang et al. 2012, 2005; Yao et al. 2009).
He et al. (2013) reported their opinion, which differs
from earlier observations. They observed that higher alka-
linity yields higher viscosity and ­OH− concentration, which
hampers the leaching of silicon and aluminum, owing to
it the geopolymerization reaction gets affected negatively.
This will further influence the mechanical properties of
geopolymers.
Zuhua et al. (2009) reported that high alkalinity depressed
the strength of geopolymers; the optimum NaOH concen-
tration is 9 M beyond which the strength of metakaolin
geopolymers decreases. The higher concentration of alka-
line solution retards the polymerization process. A higher
concentration of dissolved ions saturates the solution and
restricts the contact between the polymerized species lead-
ing to the delay in the formation of coagulated structures
(Khale and Chaudhary 2007; Liew et al. 2016).
The workability of geopolymer concrete is significantly
influenced by the concentration of NaOH. With the increased
sodium hydroxide content, the concrete mix becomes more
13

cohesive and flowability gets reduced (Chindaprasirt et al.
2007; Memon et al. 2013; Reddy et al. 2010). Metakaolin-
based geopolymer concrete shows decreased workability
with increased NaOH also because metakaolin has a high
Blaine fineness and angular shape particles (Nuaklong et al.
2018; Pacheco-Torgal et al. 2011). However, any significant
and detailed data on the study on the effect of alkali con-
centration on the workability of metakaolin geopolymers
concrete is not available.
Solids/liquids ratio
The aluminosilicate solids and liquid content of alkalis play
a substantial role in the geopolymerization process and
homogeneous mixing of ingredients in geopolymer. The S/L
ratio controls the solids and liquid content in the geopolymer
mix which directly governs the workability and geopoly-
merization reaction and ultimately influences the strength
characteristics of the geopolymer concrete (Van Jaarsveld
et al. 2002; Palomo, et al. 1999a, b).
Ramasamy et al. (2016) reported that kaolin-based geo-
polymer specimens having an S/L ratio of less than 0.6 are
failed at the curing stage due to the development of severe
cracks. Authors further reported that S/L = 0.7 is observed to
be the most appropriate ratio in terms of the hardness value.
A lower S/L ratio is responsible for the delaying of the geo-
polymerization reaction as well as lowering the workability.
Liew et al. (2012) reported that the S/L ratio affected
extremely the compressive strength of the geopolymer paste.
The S/L ratio of 0.80 resulted in the highest strength. Kong
and Sanjayan (2008) explained that the S/L ratio greatly
influences the porosity of the geopolymer paste in its hard-
ened state. At a lower S/L ratio of 0.60, many air bubbles
will be found to be entrenched into the hardened structure
which contributes to increasing porosity ultimately declin-
ing the strength.
Cheng et al. (2015a, 2015b) in their extensive study on
metakaolin-based geopolymers prepared with different S/L
ratios varying from 0.66 to 0.81 reported that porosity values
are lower with an increase in S/L ratios. The lowest value
of porosity was obtained at an S/L ratio of 0.81 along with
increased mechanical strength.
Zuhua et al. (2009) and Yao et al. (2009) used a higher
S/L ratio of 1.25 and 2.0 in metakaolin geopolymers and
observed declined value of workability. The optimum S/L
ratio for metakaolin-based geopolymers suggested by Kong
et al. (2007a, b) is 0.80 which provides optimum strength
and desirable workability. A higher value of S/L declines the
workability of the MK geopolymer paste because metakao-
lin, due to its finer particle size, has comparatively higher
water demand as comparing the other type of geopolymer.
13
Environmental Science and Pollution Research
Alkali reactant ratio
The geopolymerization mechanism in geopolymers is gov-
erned by the choice of precursors where NaOH acts as dis-
solvent and N­ a2SiO3 as a binder (Aliabdo et al. 2016; Alonso
and Palomo 2001; Granizo et al. 2004). The proportion of
NaOH and N ­ a2SiO3 solutions affects the mechanical strength
of the geopolymers (Mustafa et al. 2014). Various research-
ers conducted experimental investigations on properties of
geopolymer by varying alkali content ratios from 0.22 to
2.5 (Hardjito et al. 2004; Pelisser et al. 2013; Wang et al.
2005). Risdanareni et al. (2017) reported a poor compres-
sive strength of 4.73 MPa of geopolymer with a ­Na2OSiO2/
NaOH ratio of 2.0.
Metakaolin-based geopolymer with ­Na2SiO3/NaOH ratio
of 0.24 attained 28 days compressive strength of nearly
60 MPa (Ye et al. 2014). The geopolymer samples prepared
with a ­Na2OSiO2/NaOH ratio of 1.6 achieved compressive
and flexural strengths of 64 MPa and 17.6 MPa, respectively,
and elastic modulus of about 10 GPa which is because of
improved geopolymerization at higher alkali reactants ratio
(Pelisser et al. 2013). Villa et al. (2010) reported a similar
observation of an increase of N­ a2SiO3/NaOH ratio up to 1.5
supports the strength of zeolite geopolymers.
A general observation is with an increase in the alkali
reactant ratio up to a certain high value, the strength prop-
erties of geopolymers increased with increased N ­ a2SiO3
content polymerization process improves which leads to
improvement in mechanical strength (Pacheco-Torgal et al.
2008). A lower activator ratio is encouraged for cost-effec-
tive mix design due to the lesser cost of NaOH than N ­ a2SiO3
if workability, as well as strength, is not compromised.
Molar ratio
In a geopolymer concrete, the Na content is derived pri-
marily from an alkali solution composed of N ­ a2SiO3 and
NaOH, silica (Si), and alumina (Al) contents from alumi-
nosilicates and liquid N ­ a2SiO3. The required water con-
tent is contributed by NaOH solution, liquid ­Na2SiO3,
and extra water (if any) added during the mixing process
(Liew et al. 2016). Therefore, varying NaOH concentra-
tion, S/L ratio, and ­Na2SiO3/NaOH ratio influence the
geopolymerization process in the geopolymer system. The
usual geopolymer arrangement is commonly expressed as
­nM2O·Al2O3·xSiO2·yH2O, where M is Na or K. The amount
of Al available in geopolymer has a dominant effect on set-
ting time, the microstructure, and the strength of geopoly-
mer (Silva et al. 2007). The final setting time of geopolymer
decreased with increased Al content, i.e., on decreasing the
­SiO2/Al2O3 molar ratio which further also influences the
compressive strength.
Environmental Science and Pollution Research
In general, the Si, Al, and Na contents control the trans-
formation of the amorphous to the crystalline phase. The Si/
Al and Na/Al ratios also show great influence on the dissolu-
tion, the hydrolysis, and the condensation reaction of geo-
polymers which further controls the properties of metakaolin
geopolymer products (Liew et al. 2016).
Metakaolin is a rich source of ­Al2O3 and ­SiO2 shows high
reactivity with alkaline activators, and therefore accelerated
the geopolymerization process. The compressive strength
and the development of the microstructure of metakaolin
geopolymer largely depend on the Si:Al and Na:Al molar
ratios (Duxson et al. 2005; Rowles and O’Connor 2003; Ste-
venson and Sagoe-Crentsil 2005).
Different researchers have different opinions on Si:Al
ratios (Davidovits 1982; Komnitsas and Zaharaki 2007;
Rowles and O’Connor 2003). Davidovits recommended the
ideal ratio of N­ a2O/Al2O3 and S ­ iO2/Al2O3 as 1.00 and 4.00
respectively, to achieve high strength and durable geopoly-
mer products (Davidovits 1982).
According to D.Silva et al. (Silva et al. 2007), the
most favorable ranges of SiO2/Al2O3 and Al2O3/Na2O
are 3.4–3.8 and 0.8–1.0, respectively, particularly for the
strength development in the geopolymer systems. Provis
and Deventer (Provis and van Deventer 2007) reported that
the initial rate of geopolymerization reaction decreases with
increasing SiO2/Al2O3 ratio in the range of 2.0–3.5 before
solidification of the geopolymer paste.
Fletcher et al. (Fletcher et al. 2005) reported that with the
increase in S­ iO2 content (­ SiO2/Al2O3 = 0.5 to 1.0), geopoly-
mer structure transforms from crystalline to amorphous and
improves the mechanical properties. Silica content enhances
mechanical strength, and alumina content significantly con-
trols the setting behavior of geopolymers. Higher silica
content enhances the dissolution of aluminosilicates during
geopolymerization reaction (Dimas et al. 2009; Liu et al.
2014; Yunsheng et al. 2010).
Rowles M. and Connor O.B. (Rowles and O’Connor
2003) reported that the mechanical strength properties of
metakaolin geopolymer depend considerably on the Si:Al
and Na:Al molar ratios. The geopolymers corresponding to
Si:Al:Na ratios of 1.5:1.0:0.72, 1.5:1.0:1.5, and 2.5:1.0:1.29
achieved low, medium, and high compressive strength,
respectively. The specimens with low and medium strength
were highly inhomogeneous because of the presence of large
grains may be due to incomplete dissolution. The high-
strength material showed a more homogeneous structure.
It is concluded that on increasing Si/Al and Na/Al ratios
geopolymers get transformed into an extra homogeneous
structure.
Duxson et al. (2005) reported a linear increase in com-
pressive strength of metakaolin geopolymer with Si/Al ratio
between 1.15 and 1.90. A significant change in geopolymer
microstructure is observed between Si/Al ratios of 1.40 and
1.65 as shown in Fig. 4. A low mechanical strength was
observed in the specimen with Si/Al ≤ 1.40 because of loose
microstructure structured precipitates with large intercon-
nected pores and unreacted material. Moreover, geopolymers
with Si/Al ≥ 1.65 show a more homogeneous structure.
Lizcano et al. (2012a, b) reported that in metakaolin-
based geopolymers, the density increased with increasing
Si/Al ratios irrespective of the type of precursor but the
density of Na-activated geopolymer was lesser than that of
K-activated ones for all Si/Al ratios. The strength increased
only at lower Si/Al ratios (below Si/Al = 1.5–2). However,
at higher Si/Al ratios, all mechanical properties decrease
because solution becomes more viscous and lesser homoge-
neous microstructure with numerous unreacted metakaolin
particles, more porosity along with some microcracks.
Zhang et al. (2010) revealed that N ­ a2O/Al2O3 and H­ 2O/
Na2O significantly influence the compressive strength of
geopolymers. The highest compressive strength of 34.9 MPa
was achieved at ­SiO2/Al2O3 = 5.5, ­Na2O/Al2O3 = 1.0, and
­H2O/Na2O = 7.0. This result as indicated by IR spectra was
because the sample showed the complete geopolymerization
reaction with the largest amount of geopolymers.
Based on Juan J. et al. (Yuan, He, and Jia 2017), as
shown in Figs. 5 and 6, XRD patterns and SEM images
are illustrated. The geopolymer samples with different Si/
Al ratios show amorphous character, i.e., a broad hump at
28° 2θ. It reveals that changed Si/Al ratios did not change
the geopolymer matrix nature. The surface morphologies
of geopolymer composites showed more compactness on
increasing Si/Al from 1.75 to 2.0. There were many cracks
in the surface of the sample with Si/Al = 2.25, With the
increase in Si/Al ratio, mechanical strength increased
reaching the highest value at Si/Al = 2, and then decreas-
ing. However, there was a noteworthy decline in perfor-
mance when Si/Al = 2.25.
It is obvious from the above discussion that Si/Al ratio
and alkaline activators are the very important key parameters
that influence the geopolymer synthesis. The alkaline activa-
tor affects the dissolution of alumino-silicate raw materials
during the geopolymerization of the geopolymers. In addi-
tion to the above parameters, the presence of alkali cations
­(Na+, ­K+) is also required in the geopolymer network which
can balance the negative ions of ­Al3+ in IV-fold coordina-
tion. One mole IV-fold coordinated ­Al3+ requires 0.5 mol
of ­Na2O or K ­ 2O for maintaining the electrical neutrality to
control the rate and extent of the polymerization along with
the stabilization of the geopolymers (Davidovits 1994; Yun-
sheng et al. 2010). Therefore, to gain maximum strength
from geopolymerization, mostly researchers (Duxson et al.
2005; Subaer and Van Riessen 2007) used Na/Al = 1. For
geopolymers with Na/Al = 1, a maximum value of Si/Al can
be taken as 4.0 (Duxson et al. 2005).
13
 Environmental Science and Pollution Research

Fig. 4  SEM micrographs of Na-

geopolymers. Si/Al ratio of a
1.15, b 1.40, c 1.65, and d 1.90
(Duxson et al. 2005)

Fig. 5  XRD patterns of geopol-

ymer composites with different
Si/Al ratios (Yuan et al. 2017)

The structure of metakaolin-based geopolymers in sodium (Gao et al. 2014; Nasab, Golestanifard, and Mackenzie
silicate solution depends on the S­ iO2/Na2O molar ratio as 2015). The higher ­SiO2/Na2O ratio decreases the hardening
it affects the degree of geopolymerization of geopolymer process of geopolymer (Rahier et al. 2007). The increased

13
Environmental Science and Pollution Research

Fig. 6  Surface morphologies of geopolymer composites with different Si/Al ratios. a 1.75. b 2. c 2.25 (Yuan et al. 2017)

Fig. 7  SEM photographs

of WCMBGs with various
SiO2/Na2O ratios (curing
time = 28 days) (H. Cheng,
K.-L. Lin, et al. 2015)

­K2O or ­Na2O content accelerates the setting reaction and
strength development.
Cheng et al. (2015a, 2015b) investigated the S
­ iO2/Na2O
ratio’s influences on the mechanical properties of waste-
catalyst metakaolin-based geopolymers (WCMBG). The
microstructures study results of the geopolymers prepared
with 10% waste-catalyst replacement with different ­SiO2/
Na2O (S/N) ratios are shown in Fig. 7. The microstructure of
geopolymer specimens gets more compact with an increased
density with increased S/N ratio indicates the enhancement
of geopolymerization reaction.
Nasab et al. (2015) predicted that higher S ­ iO2/Na2O
increases the amorphous products while lower ­SiO2/Na2O
ratio showed a higher crystallization effect of zeolite mate-
rials. Based on the SEM images of metakaolin-based geo-
polymers obtained by Gao et al. (2014), the effects of the
­SiO2/Na2O ratios (1.00–2.00) on nano-SiO2 metakaolin-
based geopolymers is illustrated in Fig. 7. The setting time
of the nano-SiO2-metakaolin-based geopolymer increased

13

Fig. 8  SEM photographs of
nano-SiO2-metakaolin-based
geopolymers with various SiO2/
Na2O ratios (Gao et al. 2014)
with the ­SiO2/Na2O ratio because of the viscous property
of the sodium silicate. The SEM graphs reveal that at a high
­SiO2/Na2O ratio, homogenous geopolymer matrix is formed
which becomes denser with an increase in S/N ratio. The
structure of the geopolymer with a ­SiO2/Na2O ratio of 1.50
was more compact, had higher density, and had lower poros-
ity (Fig. 8).
The ­H2O/Na2O ratio controls the alkalinity of alkali
solution which further influences the reaction products.
Davidovits (1999), suggested the use of H ­ 2O/Na2O (10–25)
ratio, to achieve higher strength and durability properties in
metakaolin geopolymers. Barbosa et al. (2000) concluded
in their study: the optimum ratios of ­Na2O:SiO2 = 0.25,
­H2O:Na2O is 10, and S ­ iO2/Al2O3 = 3.3. The sodium content
in these ratios is sufficient to balance the charge within the
structure. They further noticed that a higher ­H2O:Na2O ratio
13
Environmental Science and Pollution Research
can form sodium carbonate which may disrupt the polym-
erization process due to which extremely low mechani-
cal strength was obtained. This statement is supported by
Ghanbari et al. (2015), in which a higher ­H2O/Na2O ratio
negatively affected the compressive strength of geopolymer
because of high porosity developed into the system due to
water withdrawal.
Kamalloo et al. (2010) obtained the highest compres-
sive strength of 80 MPa from metakaolin-based geopoly-
mers with ­SiO2/Al2O3, ­Na2O/Al2O3, ­H2O/Na2O, and ­K2O/
Na2O ratios in the range of 3.6–3.8, 1–1.2, 10–11, and 0.6–1,
respectively. Table 3 summarizes the ­SiO2, ­Al2O3, ­Na2O, and
­H2O contents that affect the properties of geopolymers. The
strength properties of geopolymers are significantly influ-
enced by varying the molar ratio of the constituent oxides.
 Table 3  Effects of molar ratios on metakaolin-based geopolymers reported in various studies
Type of study
Silva et al. (2007)
Fletcher et al. (2005)
Rowles and O’Connor (2003) Metakaolin
Duxson et al. (2005)
Lizcano et al. (2012a, b)
Yunsheng et al. (2010)
Barbosa et al. (2000)
Ghanbari et al. (2015)
Kamalloo et al. (2010)
Kong et al. (2007a, b)
13
Precursor material Molar ratios Compressive strength/days/curing temp Primary findings
SiO2/Al2O3 Na2O/Al2O3 H2O/Al2O3 H2O/Na2O
Metakaolin 3.4–3.8 0.8–1.00 – 13.6 22 MPa/3 days/40 °C The properties of a geopolymer can be
controlled by minor changes in Si and Al
content during synthesis
Metakaolin 16 5 54 11 10.9 ­MPa*/1 day/40–90 °C Geopolymer specimen get hardened at ambient
temperature; high-alumina content lowers
the strength, shows elastic behavior, and
deformed rather than brittle failure
2.5 1.29 18.01 –- 64 MPa/7 days/75 °C for 24 h The bonding network in the amorphous alu-
Environmental Science and Pollution Research
minosilicate system significantly alters with
Si:Al and Na:Al composition. The compres-
sive strength depends on the Si:Al and Na:Al
molar ratios
Metakaolin 1.9 1 1 11 80 MPa/#/40 °C for 24 h Geopolymers with a higher Si/Al ratio exhibit
reduced strength because higher silica
content results in the presence of unreacted
material in the specimens
Metakaolin 3 1 11 – 32 MPa/1 day/80 °C for 24 h Geopolymer with a higher Si/Al ratio results
in inhomogeneous microstructure with the
presence of unreacted metakaolin particles,
large pores, and some microcracks that all
result in lower mechanical properties
Metakaolin 5.5 1 7 34.9 MPa/28 days/20 °C The molar ratios of Na2O/Al2O3 and H2O/
Na2O had a significant effect on compres-
sive strength. The geopolymer possesses the
highest strength due to fully reacted material
resulting in the largest amount of geopoly-
mer gel
Metakaolin 3.3 0.83 10 10 49 MPa/3 days/65 °C ––
Metakaolin 2.9 0.84 8 13.75 66 MPa/28 days/85 °C The curing temperature and molar ratio
of H2O/Na2O have the lowest and high-
est effect on the compressive strength of
geopolymer
Metakaolin 3.6–3.8 1–1.2 11 10–11 80 MPa/7 days/70 °C for 4 h Artificial neural network optimization is in
good agreement with probabilistic values
Metakaolin 1.54 0.42 – –- 45 MPa/3 days/80 °C for 24 h The Si/Al ratio has a significant influence on
elevated temperature exposure deterioration
of metakaolin containing the potassium-
based alkaline solution. Lesser strength loss
due to elevated temperature exposure was
observed in geopolymer with high Si/Al
ratios (> 1.5)

Water content
The water content in geopolymers is categorized as free
water or physically adsorbed water and structural water.
Free water is the absorbed water and is held in macro-
pores which influence the strength and microstructure of
geopolymer paste (Davidovits 2011; Lizcano, et al. 2012a,
b; Zuhua et al. 2009), which is rigidly bound mainly by
hydrogen bonding, and is termed as structural water which
constitutes an integral part of the geopolymer matrix in
the form of molecular water. The loss of structural water
would cause the decomposition of its geopolymer structure
(Liu et al. 2016).
White et al. (2010) in their study, based on neutron pair
distribution function (PDF), reported that the majority of
the water present in metakaolin-based geopolymers is free
water which is found to have occupied the large pores in the
matrix. Most of the free water evaporates upon heating up
to 200 °C but a small amount of water, around 5% in MK
geopolymers, remains trapped within the small pores in the
framework or as terminal hydroxyl groups.
As discussed above, water is an integral part of geo-
polymers and is required during geopolymerization for the
destruction of solid particles and the hydrolysis of dissolved
Al3 + and Si4 + ions (Zuhua et al. 2009). The mineralizing
and stabilizing actions of water play important roles in disso-
lution, transport of dissolved ions, hydrolysis of oligomers,
and polycondensation of oligomers which ultimately con-
trol the formation, structure, and properties of geopolymers.
Water is even required at the end of the geopolymerization
process because polycondensation processes are associated
with dissolution (Zuhua et al. 2009).
It is a fact that water decreases the viscosity of the mix
and further enhances the flowability in fresh geopolymer
mixture. Water helps in the geopolymerization reaction by
acting as a medium for the transportation of ions (Yunsheng
et al. 2010). An excess amount of water negatively affects
the geopolymerization process by diluting the alkalinity of
reaction components and leaching away the ions from the
reaction zone (Barbosa et al. 2000).
The quantity of water required in geopolymer largely
depends on the chemical composition of the system. A lower
Na/Al ratio requires more water. The ‘‘free’’ water require-
ment was estimated as 4–6 mol per Na or K and the inter-
stitial water as 0.6–0.8 mol per Na or K. The initial reaction
water requirement varies from 3.3 to 12.5 mol per Na or K
in the literature (Perera et al. 2006).
The quantity of water present in the original precur-
sors influences the porosities in geopolymers (Perera et al.
2007). The loss of free water from pores causes drying
shrinkage which results in shrinkage cracks. Resistance to
thermal shrinkage of metakaolin geopolymers far superior
13
Environmental Science and Pollution Research
Fig. 9  Porosity accessible to water versus a the total amount of water
of geopolymer concrete (Pouhet and Cyr 2016)
to Portland cement, when exposed to temperatures above
700 °C, is in many cases (Barbosa and MacKenzie 2003b).
A comparatively higher quantity of water content during
initial mixing allows more quantity of water to get expelled
before the start of the shrinkage process (Kuenzel et al.
2012). Shrinkage is accelerated by the loss of water during
curing which leads to a reduction of strength. Therefore,
to prevent shrinkage, structural or non-evaporable water
needs to be available in the matrix which further supports
the structural stability (Kuenzel et al. 2012).
The density and open porosity of geopolymers are very
much dependent on the water content in geopolymer precur-
sors (Perera et al. 2007; Pouhet and Cyr 2016). The amount
of free water, entrapped in intergranular space, affects geo-
polymer density and porosity (Latella et al. 2008; Lizcano,
et al. 2012a, b; Zuhua et al. 2009).
Pouhet R. and Cyr M. (Pouhet and Cyr 2016) reported
that the total pore volume of metakaolin geopolymer con-
crete got increased almost linearly with the total amount of
water in the geopolymer irrespective of other parameters
such as the binder ratios or the aggregates content as shown
in Fig. 9.
Curing regime
Geopolymers are generally cured at a higher temperature
preferably lower than 100 °C. Various methods of heat cur-
ing such as steam-saturated hydrothermal treatment, elec-
tric hot air oven, and autoclave curing are in practice. Heat
curing is adopted to increase the rate of the polymeriza-
tion reaction. At higher temperatures, the dissolution of
silica and alumina species from aluminosilicates increases
which further supports the hardening of geopolymer matrix
(Alonso and Palomo 2001; Kong et al. 2007a, b; Perera et al.
2007; Yao et al. 2009). Higher temperature curing results in
high early strength but may also deteriorate the long-term
strength properties; water gets evaporated rapidly leaving
Environmental Science and Pollution Research
behind large pores which increases the tendency of cracking
in geopolymer concrete (Rovnaník 2010). To avoid cracks,
the samples should be sealed before heat curing to preserve
a small amount of structural water which is required in the
structure to avoid cracking (Van Jaarsveld et al. 2002; Liew
et al. 2016). Perera et al. (2007), suggested that crack-free
metakaolin geopolymers can be obtained at ambient and
mild heating curing in the temperature range of 40–60 °C
with controlled relative humidity. The porosity can also be
decreased by variation in the composition of geopolymers.
Metakaolin-based geopolymer concrete requires lesser tem-
perature for curing in comparison to fly ash-based geopoly-
mer concrete. A study reported that in the case of metakaolin
geopolymer concrete, an optimum range of the temperature
for curing is 32–48 °C such as exposure under sunlight or at
room temperature (Al-Shether et al. 2016b).
Tashima et al. (2013) predicted that the formation of geo-
polymer microstructure and its mechanical strength varies
with curing temperature and curing time. The SEM images
obtained showed the formation of an amorphous phase and
densification of the geopolymer matrix with the increase in
curing time. The geopolymer paste cured for 3 days at 65 °C
shows a compact-dense microstructure with an increased
amount of amorphous gel, occupying an important part of
the volume in the sample. The optimum curing time reported
was 72 h at 65 °C (Tashima et al. 2013).
The result obtained by Mo et al. (2014) reported that the
trend of rising compressive strength with curing temperature
and time indicates that the polymerization process rate of the
geopolymer is relatively slow at low temperatures. The best
curing condition they observed was 60 °C for 168 h, where
the geopolymer showed the highest compressive strength. At
higher curing temperatures (80–100 °C), the dissolution of
the amorphous structure of metakaolin particles speeds up,
a higher loss of moisture content which ultimately obstructs
the strength development. The amorphous gel phase con-
tributes significantly to the mechanical properties of alkali-
activated metakaolin-based geopolymers.
Microstructural study of metakaolin
geopolymer with different additives
Many researchers investigated the mechanical and durability
properties of metakaolin geopolymer and found them to be
of brittle or semi-brittle nature which adversely affects the
mechanical properties of metakaolin geopolymer products.
The quest to improve MK-polymer’s properties fascinated
the researchers to use different additives in MK geopoly-
mer, and in the current section, such types of research are
compiled.
Chen et al. (2018) investigated the effect of the inclu-
sion of polyacrylic emulsion (PAA) and polypropylene fiber
(PPF) in metakaolin-based geopolymers. The results showed
that the inclusion of PAA and PPF improved the mechani-
cal properties of metakaolin geopolymers (MKG). The flex-
ural strength, the ratio of compressive strength to flexural
strength (F/C), and the flexural toughness can suitably be
enhanced with apt additions of PPF and PPA. The micro-
morphology photographs of polypropylene fiber MKG sam-
ple taken from the paste after the failure of fiber-MKG are
compared with PF-MKG containing 5 wt% of polyacrylic
emulsion. It can be seen in Fig. 10 that the polymer addi-
tion improved the interfacial adhesion between the fiber and
matrix. In Fig. 10a-1 (MKG with PPF), the surface of the
pulled-out fiber is seen to be quite smooth in comparison
to fiber visible in Fig. 10b-1 (MKG with PAA and PPF). In
Fig. 10b-1, a fraction of the paste is seen to be attached to
the fiber after failure.
SEM graphs show the presence of a layer of organic poly-
mer gel ( can be seen as a high amount of carbon content
near Spot 1 and lower content of silicon and aluminum).
Whereas near Spot 2, carbon content is low and silicon and
aluminum contents are high, which are further verified by
the EDS graphs in Fig. 10b-2. Hence, it indicates that PF-
MKG with fibers and organic polymers shows better flexural
strength and flexural toughness.
Logesh Kumar and Revathi (2020) used bottom ash in
alkali-activated metakaolin and study the microstructural
properties of the composite. The authors observed MK-
GPC gained higher compressive strength in comparison
to OPC-concrete. The inclusion of bottom ash resulted in
significantly higher compressive strength which is due to a
significantly more effective geopolymer reaction between
metakaolin and bottom ash.
Kalaiyarrasi and Partheeban (Kalaiyarrasi and Parthee-
ban 2019) reported their study on mechanical and micro-
structural properties of metakaolin (MK)-based geopolymer
with fly ash (FA). Various proportions of MK and fly ash
were taken for investigations. MK-added fly ash geopoly-
mer showed enhanced compressive strength in comparison
to fly ash geopolymer. It can be analyzed from SEM pic-
tures of metakaolin GP ( 50% MK + 50% FA) with different
types of MK precursors such as M2 and M3 with increas-
ing ­SiO2 and decreasing Al2O3 contents, respectively, as
shown in Fig. 11. Microstructure in Fig. 11b shows a more
compact structure in comparison to Fig. 11a which reveals
that MKGPC has better mechanical properties and compact
microstructure which can further also be improved with
increasing the SiO2 content. It is also mentioned that Al2O3
present in the aluminosilicate only initiated the reaction but
does not contribute to any strength. However, the enhanced
compactness of the matrix improves the durability proper-
ties of MKGPC.
13
 Environmental Science and Pollution Research

Fig. 10  Scanning electron microscopic (SEM) images of a metakaolin geopolymer with PPF and b metakaolin geopolymer with PAA and PPF;
EDS Spot1 and Spot2 (Chen et al. 2018)

Applications of MK‑based geopolymers significantly higher acid and fire resistance. Researchers
showed that geopolymers can be used in various applications
Geopolymers possess excellent properties including such as in materials used for protective coating of different

13
Environmental Science and Pollution Research
Fig. 11  SEM images of the
a 50% metakaolin + 50% fly
ash, M2 precursor and b 50%
metakaolin + 50% fly ash, M3
precursor (Kalaiyarrasi and
Partheeban 2019)
surfaces including metals, as sustainable concrete, fireproof
building materials, and environmentally friendly materials
due to their superior mechanical, chemical, and thermal
resistance properties. The section summarizes the potential
applications of geopolymer cement and concrete.
Anti‑corrosion products
The unique 3-D network structure of geopolymeric gels
and the presence of very low calcium hydroxide content
result in better anti-corrosion properties than conventional
Portland cement-based products (Zhang, Yao, and Zhu
2010). Geopolymers may also be custom-made to be used
as a primer or textural paint for different surfaces. Geopol-
ymer cement showed relatively higher adhesive strength
with steel, aluminum, and borosilicate glass (Bell et al.
2008). The adhesive strength of the geopolymer coating
to steel strongly depends on the chemical composition of
the coating material.
Zhang et al. (2010) investigated the resistance to tide
wave shock on geopolymer coating applied in situ on con-
crete surfaces in the coastal area. They reported a strong
bond of coating with concrete along with a good resist-
ance was offered to tidal waves within 4 h. Furthermore,
polypropylene fibers and a small amount of magnesium-
based expansion agent when used, large shrinkage problem
has successfully decreased the shrinkage to an acceptable
level.
Therefore, geopolymers can be used as an anti-corrosion
protective layer on metal surfaces and marine concrete to
prevent corrosion and also to improve appearance, wear
resistance, scratch, and also its thermal resistance properties.
Thermal resistant and fireproof material
Many researchers investigated the scope of geopolymers’
application as thermal and fire-resistant materials. Kong
et al. (2007a, b) reported that metakaolin-based geopolymers
when exposed to higher temperatures showed a decrease in
strength which may be due to higher water loss in compari-
son to fly ash-based geopolymers.
Temuujin et al. (2009) reported the high-water resist-
ance and fireproof properties of coating material prepared
by geopolymer based on metakaolin. This fireproofing coat-
ing material forms a layer that is heat-insulating, resulting in
creating a protective atmosphere. The endothermic processes
further lower the surface temperature. Metakaolin exhibits
expansion with the formation of a porous structure which
may act as a thermal barrier between the coating material
and the metal surface. In another study, authors (Temuujin
et al. 2010) reported that the best adhesive strength can be
achieved for geopolymers containing high silica composi-
tions. Increasing coating thicknesses will further enhance
the fire-insulating capacity.
Bo and Shuai (2011) reported that carbon fiber reinforced
metakaolin-based geopolymer results in higher strength con-
crete of 51.2 MPa at the age of 28 days.
Metakaolin-based geopolymer containing an ­H2O/Al2O3
ratio of 13, remains structurally stable when exposed to
600 °C (Zhu et al. 2013). Hung et al. (2013) synthesized a
metakaolin-based geopolymer mixture of 70% metakaolin
and 30% blast furnace slag powders activated with alkaline
activating solutions. The coefficients of thermal conductivity
of the specimens so produced using a mechanical foaming
process were lower than 0.1 W/m°K when its relative den-
sity is reduced to lesser than 0.2.
Wu et al. (2014) investigated the properties of fireproof
coating ( up to 10 mm) prepared with rice husk ash and
alkali-activated metakaolin geopolymer as main raw mate-
rials on demolished concrete blocks. The thermal conduc-
tivity of the fireproof coating was measured at room tem-
perature. The influences of the demolished concrete blocks
( DCBs), load ratio, and thickness of the fireproof coating
on the fire resistance of the composite slabs were examined.
They reported that fireproof coating has exceptional thermal
insulation properties, and in the case that the geopolymer
binder is activated by sodium silicate.
13

Sakkas et al. (2014) prepared metakaolin geopolymer
doped with solid ­SiO2, activated by the highly alkaline
potassium hydroxide solution. They reported the metakao-
lin geopolymer to possess excellent fire-resistant properties
along with lower thermal conductivity. The material so pre-
pared can be better used as an effective heat flux barrier and
find its application in fire protection cover to the tunnel’s
concrete linings from the most severe fire incidents.
Duan et al. (2015) revealed in their study that the micro-
structures of fly ash-metakaolin-based geopolymer paste
showed increased densification with the increase in fire
temperature up to 400 °C because of sintering and further
geopolymerization with the increase in temperature. Geo-
polymer concretes are suitable for thermal applications up
to 1100 °C (Kamseu et al. 2010).
Rashad (2019) reported that the MK-based geopolymer
mortars displayed enhanced fire resistance in the ranges of
10.25–11.58% higher relative strength in comparison to the
fly ash-based mortars. The fly ash-based geopolymer mor-
tars instead showed higher thermal insulation (12.9–38.33%
lower thermal conductivity) than the metakaolin-based geo-
polymer specimens. Further higher thermal insulation and
better fire resistance can be achieved by replacing siliceous
sand with expanded perlite as fine aggregates.
On the contrary, Rovnanik and Šafránková (2016)
reported a considerable deterioration in the mechanical
properties of metakaolin-based geopolymer when subjected
to a temperature of 1200 °C which was further improved
with the addition of chamotte aggregate. Metakaolin geo-
polymer mortar with chamotte aggregate showed much
higher strength. In general, metakaolin-based geopolymers
can be presented as promising products for high-temperature
applications.
Discussions
During the review of the available literature, it is observed
that metakaolin which is obtained from the calcination of
kaolin at a higher temperature in the ranges of 550–750 °C
is a long back in practice as an admixture in concrete to
enhance its properties. Studies reported it as the most widely
used aluminosilicate material. The increase in the amor-
phous phase of metakaolin in comparison to kaolin favored
the higher degree of polymerization which is the backbone
of the strength properties of geopolymeric products such as
geopolymer paste, mortar, and concrete.
A deep insight into the research available so far indicates
that metakaolin-based geopolymers due to their lower den-
sity can be better used as a lightweight concrete (having
bulk density = 2.10 to 2.40 g/cm3) which further decreases
with higher curing temperature (below 60 °C); however, at
curing temperature more than 60 °C, it negatively affects the
13
Environmental Science and Pollution Research
physical properties due to rapid setting. Many authors are of
opinion that the addition of small quantities of nanomateri-
als, such as nano-silica, nano-sand, and nano-clay, is quite
helpful in increasing the compressive strength of metakaolin
geopolymers. However, sufficient literature is not available
which can emphasize the experimental findings related to
durability properties of metakaolin geopolymer concrete
which may be considered as a research gap for prospective
researchers.
Metakaolin geopolymer due to its 3-D network of geopol-
ymer gels as well as possesses lesser calcium oxide content
may be proved to be good in the applications of anti-cor-
rosion materials. Metakaolin-based geopolymers may also
find a good place as high-water resistance and fireproofing
coating materials. These materials form a good heat-insulat-
ing layer which shows an endothermic effect and lowers the
surface temperature of the structure where it is used.
Conclusions and future scope of the study
An emphasis is done to compile the information available
in the research field on metakaolin-based geopolymers, and
based on the detailed discussion so far, the following conclu-
sions are drawn.
1. Metakaolin is a unique type of pozzolanic material and
can be obtained from clay by the process of calcination
and shows very satisfactory performance in geopolymer-
based products too similar to conventional concrete.
2. The strength of metakaolin geopolymers is largely influ-
enced by the NaOH concentration, which is observed to
be 9 M as optimum. At a higher NaOH concentration
due to increased alkalinity, the polymerization process is
suppressed and adversely affects the strength properties.
3. Aluminosilicate solids to liquid ratio and alkali reactant
ratio significantly influence the properties of metakao-
lin-based geopolymers. The S/L ratio ranging between
0.6 and 0.8 is found to be resulting in better strength
as well as reduced porosity. A lower S/L ratio than 0.6
adversely affects the porosity due to the development of
air bubbles. A higher value of S/L results in decreased
workability due to the higher water demand of metakao-
lin particles.
4. Similar to other types of geopolymer concrete, metakao-
lin GPC is also greatly influenced by the curing tempera-
ture. The optimum temperature for curing metakaolin
geopolymer concrete is found to be lesser than 60 °C.
5. Metakaolin-based geopolymer products are much bet-
ter than other types of geopolymers due to their better
water resistance, good fireproof resistance, and suitable
corrosion resistance abilities. However, more detailed
Environmental Science and Pollution Research
research on durability properties may pave the path for
the commercial success of MK-based geopolymers.
Data availability and materials
Not applicable.
Author contribution Bharat Bhushan Jindal: conceptualization, inves-
tigation, data analysis, writing—original draft, writing—review and
editing.
Thamer Alomayri: writing—original draft, reviewing.
Assaedi Hasan: writing—original draft, reviewing, editing and
proof reading.
Cyriaque Rodrigue Kaze: writing, proof reading, grammer,
reviewing.
Declarations
Ethics approval and consent to participate Not applicable.
Consent for publication Not applicable.
Conflict of interest The authors declare no competing interests.
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