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Recent Progress in Environmentally Friendly Geopolymers A Review
Recent Progress in Environmentally Friendly Geopolymers A Review
Recent Progress in Environmentally Friendly Geopolymers A Review
PII: S0048-9697(20)36696-1
DOI: https://doi.org/10.1016/j.scitotenv.2020.143166
Reference: STOTEN 143166
Please cite this article as: N. Shehata, E.T.S. Ali and M.A. Abdelkareem, Recent progress
in environmentally friendly geopolymers: A review, Science of the Total Environment
(2020), https://doi.org/10.1016/j.scitotenv.2020.143166
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of
emissions of CO2 resulting from the decomposition of limestone that consequently resulted in
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severe environmental impact that is estimated by one ton of CO2 per ton of cement.
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Geopolymerization technology is an effective method for converting wastes (containing alumina
and silica) into useful products. It can reduce CO2 emissions significantly from the cement
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industry. The geopolymerization process usually starts with source materials based on
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alumina/silicate in addition to alkaline liquids. The compressive strength, setting time, and
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workability of the final product depends mainly on the type and proportions of the precursors,
the type and strength of the activator, the mixing and curing conditions. The structural
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geopolymer can replace OPC, and thus decreasing the energy consumption, reducing the cost of
the building materials, and minimizing the environmental impacts of the cement industry. This
and different raw materials (fly ash, kaolinite and metakaolin, slag, red mud, silica waste, heavy
metals waste, and others) with particular focus on recent studies and challenges in this area.
1. Introduction
Since the industrial revolution in the last century, there is a rapid growth of the usage of
fossil fuel in almost all industrial applications (Shafeek et al., 2020). Such an increase in the
usage of fossil fuel resulted in severe environmental impacts (Abdelkareem et al., 2020a;
Elsaid et al., 2020c, 2020b, 2020a). Massive efforts have been done to minimize the
environmental impacts of fossile fuel such as increasing the efficiency of the current processs
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(Elsaid et al., 2020d; Fierro et al., 2020; Jouhara et al., 2018; Olabi et al., 2020a; Shehata et
al., 2017), development of efficient energy conversion devices suh as fuel cells
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(Abdelkareem et al., 2020b, 2020c; Olabi et al., 2020b; Sayed et al., 2020b), hybrid systems
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of renewable energy systems (A Kamel et al., 2019; Rezk et al., 2019b), and/or using of
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renewable energy sources such as wind, solar (Abdelkareem et al., 2018; Marmoush et al.,
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2018; Rezk et al., 2019a), geothermal (Wilberforce et al., 2019a), marine (Soudan, 2019),
The cement industry is one of the leading sectors that consume a large amount of fossil fuel
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that estimated to be 12-15% of the industrial energy consumption (Madlool et al., 2011). A
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massive amount of pollutants such as CO2, CO, NOx, SO2, and particulates are emitted from
the cement industry from fossil fuel and the decomposition of the limestone (Ekinci et al.,
2020). The emitted CO2 from the cement industry represents 5-8% of the anthropogenic CO2
emissions (Deja et al., 2010; Shen et al., 2015). CO2 is one of the major greenhouse gases
that resulted in global warming and noticeably environmental changes overall the world
It is estimated that each ton of cement produces 498.5 kg of CO2 that resulted in more than 2
Gt of CO2 production overall the world (Wei and Cen, 2019) that is increased exponentially
with the exponential increase of the cement production overall the world (Xu et al., 2015).
There are common methods that were investigated to decrease the CO2 emission during
cement production, like the use of alternative fuel (El-Salamony et al., 2020), enhancement
of energy efficiency inside the cement kiln (Hasanbeigi et al., 2013), replacement the cement
with nanoparticle at the optimum percentage (Shafeek et al., 2020) and production of
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alternative cement-like geopolymer (Bajpai et al., 2020). Still, the production of geopolymer
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superior to all methods since it represents a high reduction in cost (Amran et al., 2020) and
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energy consumption (Voney et al., 2020), besides the added benefit of using industrial wastes
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to develop a different building material (Tong, 2020). Consequently, there is an increase
focus on the geopolymer studies all over the world as shown in Fig. 1.
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7000
6000
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No. of scientific papers
5000
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4000
3000
2000
1000
0
2010 2011 2012 2013 2014 2015 2016 2017 2018 2019
Year
Fig. 1: Number of published papers related to geopolymer during the period 2010-2019.
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background of geopolymerization (Aleem and Arumairaj, 2012a; Shubbar et al., 2020) and
characterization (Damilola, 2013; Ma et al., 2018; Mo et al., 2016; Shuaibu, 2014; Zhang et al.,
2018; Živica et al., 2015), effect of synthese parameters (Farhan et al., 2020), additives (Ranjbar
and Zhang, 2020) on the final products and sustanbility (Assi et al., 2020). Still, the literature
missed discussing new precursors such as fly ash-based geopolymers (Abdullah et al., 2011; Al
Bakri et al., 2013a; Bouaissi et al., 2018; Fauziah et al., 2018; Ibrahim et al., 2015; Kupaei et al.,
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2013; Mustafa et al., 2011; Toniolo and Boccaccini, 2017; Wattimena et al., 2017; Zerfu and
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Ekaputri, 2016; Zhuang et al., 2016) that studied extensively in recent years, activators, and their
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role in the geopolymerization process, as well as the challenges for the production of geopolymer
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on a large scale, needs to be addressed. Subsequently, this review summarized different
traditional and new precursors for geopolymers, important parameters of geopolymerization, and
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new additives. Moreover, the challenges of the large scale production of the geopolymers are
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2. Geopolymerization
The manufacturing of cement demands the burning of vast quantities of fuel, as well as
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significant emissions of CO2 resulting from the decomposition of limestone (Kong and Sanjayan,
2008). According to Kong et al., geopolymer minimize CO2 emissions from the cement industry
by 80% (Kong et al., 2006). A study conducted in Lebanon around Chekka town discovered that
the cement industry was adversely affecting the overall health of the region. Elevated levels SO 2
and PM10 (Particulate matter) were found in various areas around the town for extended periods
of time. On the other hand, the treatment costs of industrial waste disposal are expensive.
immobilization agent for industrial waste. The term geopolymer refers to the inorganic polymer
followed by specific conditions of curing (Fig. 2). The following sections discuss the recent
1. Aluminosilicate precursors
2. Activators
Mixing Curing Geopolymer
3. Water
of
4. Additives
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Fig. 2: A schematic flow diagram for the geopolymer production.
addition to alkaline liquids. The precursors were classified (reticulate Blanco, n.d.) into fly ash-
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(Izquierdo et al., 2009), slag-, rock- (Gimeno et al., 2003), and Ferro silicate-based geopolymer.
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The precursors could be natural minerals such as kaolinite and clays or by product materials like
slag, fly ash, rice-husk ash, silica fume, and metakaolin (Rangan, 2008). Theses precursors can
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be a single material or a mixture of different types of materials (Xu and Van Deventer, 2002).
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However, it should be rich in silicon and aluminum (Chawakitchareon and Veesommaia, 2013).
The strength of a geopolymer depends on the nature of precursors (Duxson et al., 2007). For
example, higher compressive strength might be obtained when raw materials were calcined, such
as fly ash, slag, and metakaolin, or when it has a high dissolution rate (Rangan, 2010). The
coordination number of aluminum in the precursor may affect the final product (Rangan, 2010;
Singh et al., 2001). Calcium silicate enhances the dissolution of alumino-silicate from fly ash
structure; also, it merged in the geopolymer matrix acting as counter‐balancing cations (Horsley
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et al., 2015). Sodium aluminate increases the compressive strength twice as much as non-sodium
aluminate (Svingala and Varela, 2009). As shown in Table (1), the compressive strengths of the
final samples are influenced by the proportions and properties of the precursors.
Table 1: Composition of different types of precursors and the compressive strength of the relative
geopolymers.
of
SiO2 Al2O3 CaO MgO Fe2O3 Na2O K2O Other strength
(MPa)
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Callide 46.2 26.5 9.9 1.2 8.5 0.3 0.6 6.8 54 (VAN
Eraring 67.8 21.6 1.7 0.4 3.0 0.1 1.2 4.2 17 DEVEN
Bayswater
Vales Point
62.9
65.0
24.9
20.3
<0.1
5.6
1.0
0.9
5.2
4.5 -p
0.2
0.5
1.3
1.7
4.5
1.5
41
*
TER,
2009)
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Mount Piper 68.5 23.5 0.4 0.3 1.6 <0.1 2.3 3.4 *
Gladstone 47.5 33.2 2.6 1.8 10.2 <0.1 0.2 4.5 72
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2013)
Mine tailings 69.55 12.63 0.69 0.33 0.87 1.98 3.1 10.87 0.5-7 (Qiu et
Blast furnace 0.1 al.,
34.60 12.11 39.5 9.23 0.11 0.35 3.89
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slag 9 2019)
1.1
Fly ash 54.79 23.57 3.17 1.12 0.03 0.31 15.87
2
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In the following sections, we will discuss in detail the influence of the essential geopolymer
precursors.
The main constituents of fly ash are silicon, aluminum, calcium, and iron. The chemical
composition of various fly ash types was reported (Lloyd and Rangan, 2009). Due to its
pozzolanic characteristics, fly ash has been used as a precursor for cement and concrete (Thakkar
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et al., 2014). The calcium percentage in fly ash plays an important role, as it affects the product
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properties (Oh et al., 2010). Also, when this percentage increased, the compressive strength
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increases (Canfield et al., 2014). On the other hand, the calcium compound percentage reduces
the mechanical properties of geopolymers cured at higher temperatures (Temuujin et al., 2009).
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Usually, fly ash requires thermal treatment at 60-80°C (reticulate Blanco, n.d.). Using 5% up to
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10% of fly ash instead of Ground Granulated Blast Furnace Slag (GGBS) improves the
mechanical properties and microstructure of the produced geopolymers. More than this
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percentage, a slight decrease in the compressive strength values were measured (El-Gamal and
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Selim, 2017). Diaz et al. studied an experimental program on the mechanical properties of
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geopolymer concrete using two types of fly ash collected from thermal power stations (Diaz et
al., 2010). The compressive and flexural strengths of geopolymer based on mettur fly ash was
greater than that based on tuticorin fly ash (Vijai et al., 1970). The main characteristic of fly ash
based geopolymer is a glassy amorphous product (Fig. 3), some of the original constituents like
fly ash dissolute, leaving these pores, and it may be attributed to air involved during preparation
(Škvára et al., 2005). Kong et al. found that fly ash pores contain a higher proportion of
microspores resulting in geopolymer possess better strength (Kong et al., 2007). Improvement of
strength, workability of different geopolymers synthesized from fly ash have also been
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investigated (Adam, 2009; Chindaprasirt et al., 2007; Hardjito et al., 2004; Thokchom et al.,
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Fig. 3: SEM photos of geopolymer (Škvára et al., 2005).
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and Zaharaki, 2007). This will yield a weak structure geopolymer. Also, the contact time should
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be enough to produce the right gel components (Xu and Van Deventer, 2002). However, when
kaolinite converted to metakaolin, compressive strength and durability of the geopolymer were
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increased (Damilola, 2013). Gougazeh compared between different types of metakaolin. It was
found that Jordanian and mixed metakaolin produced the larger compressive strength compared
to others (Gougazeh, 2013). Also, it was suggested that geopolymer may still be produced from
kaoline with purity 70% (Zibouche et al., 2009). In contrast, Alshaaer et al. investigated the
characteristics from low purity kaolinite (Alshaaer et al., 2015). Douiri et al. characterized
Geopolymer
(28 d)
Counts
Geopolymer
(7 d)
of
Metkaolin
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2 Theta (degrees)
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Fig. 4: XRD spectra of metakaolin and geopolymer at curing ages (7 and 28 d) where Q: SiO2, I:
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illite, A: AlPO4, Au: Al2(PO4)(OH)3 and M: CaPO3(OH) (Douiri et al., 2016).
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Calcination of kaolinite before geopolymerization has attracted some researchers. They worked
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in almost the range (500-800 ˚C), i.e., 500- 750 ˚C (Chareerat et al., 2006; Cioffi et al., 2003),
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750 ˚C (Alshaaer et al., 2015), 800 ˚C (Zibouche et al., 2009), and concluded that the optimum
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calcination temperature is between 500 and 700˚C. This may be attributed to varying state of
disorder with calcination temperature (Elimbi et al., 2011). Another parameter that should be
taken into consideration during applying metakaolinite is the ratio of Si/Al. The amount of
unreacted kaolinite in the final matrix depends on this ratio (Fig. 5) (Kim, 2012).
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45%
40%
35%
Unreacted MK
30%
25%
20%
15%
10%
5%
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1 1.1 1.2 1.3 1.4 1.5 1.6 1.7
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Si/Al Ratio
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Fig. 5: Effect of Si/Al ratio on the percentage of unreacted metakaolinite in the geopolymer matrix (Kim,
2012).
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2.1.3. Slag
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Thakkar et al. used slag as a precursor for geopolymers (Thakkar et al., 2014). Ground
Granulated Blast Furnace Slag (GGBFS) enjoys some latent hydraulic characteristics resulting in
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using it as a common precursor. Vignesh and Vivek replaced low calcium fly ash with slag. They
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observed that the maximum compressive-, split tensile- and flexural- strengths were obtained
when the ratio of GGBS/flyash was 2/3 (Vignesh and Vivek, 2015). Some studies founded that
workability and compressive strength also increased (Saranya et al., n.d.). On contrast to other
studies that stated that replacing GGBS with fly ash resulting in an increase in compressive
strength (Fig. 6) (El-Gamal and Selim, 2017). This difference in results can be attributed to the
fact that the compressive strength and other mechanical properties depend not only on the
percentage of slag but other parameters like activator, curing regime, etc.
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20 3d
7d
28 d
10
0
A1 B1 C1
of
Geopolymer grade
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Fig. 6: Compressive strength of different specimen at 3,7, and 28 d of curing time where A1(100%
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GGBS), B1 (95% GGBS + 5% fly ash), and C1(90% GGBS+ 10% fly ash) (El-Gamal and Selim, 2017).
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2.1.4. Water
Water content is very important in geopolymerization. Also, the mechanism that water leaves the
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mixture during curing has a significant effect on the chemical/mechanical properties of the
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geopolymer produced (Barbosa et al., 2000; Rangan, 2008). The presence of excessive water
may compromise the compressive strength of geopolymer concrete (Lloyd and Rangan, 2010).
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As seen in Fig. (7a), as the water % increased, the compressive strength decreased (Patankar et
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al., 2013). In contrast to workability, where the later increased as the water % increased (Fig.
7b).
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(a) (b)
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Fig. 7: Effect of water % on compressive strength (a) and flow (b) of geopolymer concrete (Patankar et
al., 2013).
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Yong Cui and Dongmin Wang (2019) stated that the percentage of water affect the distribution
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of pore-size (Cui and Wang, 2019), as water % increased, the pore size and percentages of
Fig. 8: SEM photographs for the effect of water % on the pore structure of FA-based foam geopolymers
where water percentage ranged from 0.38 (a), 0.44 (b), 0.50 (c) (Cui and Wang, 2019).
They attributed to increasing the percentage of bubbles filled with water inside the geopolymer
paste while the viscosity of the mix and foaming agent led to prevent accumulation of small
bubbles to become large and led to declining in artificial air-pores. The water percentage should
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be optimized.
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2.1.5. Others
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Precursors like silica waste and pure alumina have been used (Chawakitchareon and
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Veesommaia, 2013). Dried red mud has been used to compensate the alkaline activator, aiming
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to lower overall costs (Horsley et al., 2015). The addition of trass reduces geopolymer concrete
strength, almost 36% of geopolymer concrete strength. This may be attributed to the content of
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silica compared to alumina, resulting in some silica will remain unreacted with NaOH
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(Risdanareni and Ekaputri, 2015). Kinnunen et al. turned rock wool waste into geopolymer with
strength 12.8 MPa using mixing and dissolution techniques; the percentage of the waste in the
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final geopolymer matrix was 33% (Kinnunen et al., 2017). Elijah (2015) optimized the addition
of mineral wool to the geopolymer; he concluded that the highest compressive strength obtained
when the percentage of mineral wool and rock wool in the geopolymer matrix were 20 and 50%,
respectively (Elijah, 2015). Commercial phosphoric acid was investigated as an activator instead
of an ordinary alkaline activator. The resulted geopolymer contains two networks, the first one
based on phosphate/aluminum, which dispersed on the second one based on Si-Al-P (Zribi et al.,
2020). The wastes from the aggregate industry were also used to produce geopolymer bricks.
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The compressive strength reached 75 MPa, parameters like the incorporation of Ca(OH)2 and
increasing curing temperature up to 105 °C played significant roles in this concern (Madani et
al., 2020).
sodium/potassium hydroxide and sodium/potassium silicate (Cioffi et al., 2003; Gougazeh, 2013;
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Komnitsas and Zaharaki, 2007; Risdanareni and Ekaputri, 2015). The aim of adding the latter is
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to improve the formation of geopolymer precursors (Xu and Van Deventer, 2000). It contains
partially polymerized silicon, which facilitates the reaction (Komljenović et al., 2010). And
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fasten the geopolymerization (Srinivasan and Sivakumar, 2013).
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The kind of alkali activators affects the solubility of the precursors (Rattanasak and
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Chindaprasirt, 2009) and determines the pore size of the final product (Damilola, 2013). The
composition, structure, microstructure, and properties of the polymers formed in the alkali
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activation of metakaolin depend on the concentration, volume and type of activator used
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(Barbosa et al., 2000), (Steveson and Sagoe-Crentsil, 2005), (Duxson et al., 2005). The increase
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in mass and the concentration of the alkaline solution strengthen the bond between the aggregate
and the binder resulting in high stiffness in the matrix (Fig. 9) (Barnard, 2014).
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of
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Mass of NaOH/m3 (kg)
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Fig. 9: Effect of alkaline solution concentration on modulus of elasticity (Barnard, 2014).
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Other researchers found that the compressive strength of the geopolymer increased when the
molarity of NaOH solution increased (Fig. 10) (Mishra et al., 2008), (Madheswaran et al., 2013),
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(Cheema et al., 2009). Concerning compressive strength, the optimum concentrations of NaOH
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activator were reported by many researchers 10M (Alonso and Palomo, 2001), (Rattanasak and
Chindaprasirt, 2009), 12 (Nazari et al., 2011), and 16M (Ramujee, 2014). Concerning setting
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times, the optimum concentration of NaOH activator was 12M-14 M (YellaIah et al., 2014). The
higher value of pH of the alkali activators enhanced the dissolution of the precursors, fasten
monomer condensation and encourage geopolymer production (Hardjito et al., 2003). As seen in
Fig. (11), the cost of the activator plays an important role among the geopolymer precursors
(McLellan et al., 2011), dry activator (sodium carbonate/ calcium hydroxide/pirssonite), was
proposed for the sake of cost reduction, NaOH solution was mixed with calcium carbonate, then
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the mixture was dried at 80 ˚C for 8 h followed by pelletizing (Abdel-Gawwad and Abo-El-
Enein, 2016).
It was found that Na2SiO3 accelerates geopolymerization process and increases the compressive
strength (Parthiban et al., 2013). Dutta & Ghosh studied the influence of Na2O on the
the increment in Na2O weight percentage (Dutta et al., n.d.). Some researchers studied the effect
of another activator-like KOH on the mechanical properties of geopolymer. They found that gain
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in strength is acceptable at 12M (Raijiwala et al., 2012). Finally, the highly reactive alkaline
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solution governs the geopolymerization process (Gharzouni et al., 2015).
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20
of
0
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M20 M25 M30
Geopolymer grade
-p
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60
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Compressive strength (Mpa)
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40
(b) 8M
12 M
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20 12 M
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0
M20 M25 M30
Geopolymer grade
Fig. 10: Effect of NaOH molarity on the compressive strength of three grades of fly ash-based
geopolymers at 3d (a), and 28d (b) (Bidwe and Hamane, 2015).
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600
500
Cost of feedstock ($/t)
400
300
200
100
of
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Fig. 11: Market price of the geopolymer precursors (McLellan et al., 2011).
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2.3. Parameters of geopolymerization process
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2014). High compressive strength was achieved when the molar ratio silicate/sodium was 1.5,
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when the ratio increased to 1.91, the compressive strength decrease (Guo et al., 2010). Because
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this high mole ratio is resulting in precipitation of Si and reduction of the compressive strength
(Dai et al., 2013). Alshaaer et al. successfully produced geopolymer using SiO2 in sodium
silicate solution/ Na2O in alkaline activators/Al2O3 molar ratio of 1/1/1 (Alshaaer et al., 2015).
The high compressive strength of Na2O/fly ash ratio was 0.1 (Guo et al., 2010), up to 0.40; after
that ratio, the compressive strength decreases (Hardjito et al., 2008). Chawakitchareona and
(Chawakitchareon and Veesommaia, 2013). Zhang et al. (2010) studied two different precursor
ratios (Al2O3/Na2O & Na2O/H2O). The highest compressive strength was achieved when
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Al2O3/Na2O is 1.0, and Na2O/H2O is (1/7) (Zhang et al., 2010). Abdul Aleem and Arumairaj
suggested an optimum mix ratio when the activator solution (NaOH & Na2SiO3) to fly ash ratio
was 0.35 (Aleem and Arumairaj, 2012b). Abdel-Gawwad& Abo-El-Enein (2016) showed that
the optimum percent of NaOH activator to blast-furnace slag is 4/100 (Abdel-Gawwad and Abo-
El-Enein, 2016). The fly ash/slag ratios were varied from 90/10, 70/30, and 50/50. The mix with
50:50 ratio shows higher compressive strength than that of the normal control concrete under
heat curing. While the other ratios show low strength at both ambient and oven curing (Thakkar
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et al., 2014). Even the shrinkage behavior of the geopolymer governed by the Si/Na ratio of the
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activator (Kani and Allahverdi, 2011). Finally, the optimum ratio of the precursors to the alkali
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should be >1. Below this value, the compressive strength will be affected negatively.
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2.3.2. Mixing regime
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Rattanasak proposed two mechanisms of mixing; normal (the two activators solutions added at
the same time) and separate mixing (a sufficient period of time was allowed for the addition of
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the two different solutions). The results showed that separate mixing is better than normal
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mixing. The separate mixing also was preferred in the case of precursors and activators (Cheng
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and Chiu, 2003; Swanepoel and Strydom, 2002). Where the activator is added later to the
precursors, the controlling parameters were related to the materials reactivity, the activator
strength, and the contact time (Mikuni et al., 2007; Panagiotopoulou et al., 2007). Also, the
mixing regime is important in case of adding fiber to the mix. It may be added to the dry
precursors like carbon and steel fiber (Ganesan et al., 2015; Vaidya and Allouche, 2011), or it
may mix with the alkaline solution first before mixing with dry precursors to facilitate its
Heat treatment must be applied to facilitate geopolymerization process, increase the reactivity of
the precursors (Ramujee, 2014), increase the compressive strength (reticulate Blanco, n.d.),
avoid the strength at delayed age (Kirschner and Harmuth, 2004), and improved the crystallinity
of the geopolymer (Dimas et al., 2009). A variety of temperatures has been investigated with a
strength, especially in the case of unmodified precursors (Swanepoel and Strydom, 2002). This
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can lead to material shrinkage (Kirschner and Harmuth, 2004), due to the evaporable water in the
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raw material that increases with the Si/Al ratio of the geopolymer (Damilola, 2013). With curing
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temperatures ranging from 60 to 90 ˚C and a time range from 24 to 72 hours, the compressive
strength of concrete reached high values (Hardjito et al., 2008). An optimum values of 60 ˚C
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(Nasvi et al., 2012) and 80 ˚C (Nazari et al., 2011), (Raijiwala et al., 2012) were suggested.
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When the temperature raised up to 100 ˚C, the hardening was accelerated, and more strength was
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gained (Alonso and Palomo, 2001). Curing at 75 ˚C for 4 hours resulted in satisfactory
properties of the geopolymer (Kirschner and Harmuth, 2004). Curing at elevated temperature
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under a long time did not improve the strength of the geopolymer (Kong et al., 2006), also rapid
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curing effects negatively on the physical properties of geopolymer (Van Jaarsveld et al., 2002).
Some geopolymer systems may be cured at room temperature using calcined precursors such as
metakaolin (Davidovits, 2008), and kaolinite (Davidovits, 1994) which gain compressive
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Fig. 12: Effect of setting time at room temperature on compressive strength of geopolymer (Davidovits,
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1994).
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However, when kaolinite are subjected to intensive thermal treatment (730-850 ˚C), it will
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transform to disordered metakaolin, which enhances its subsequent reactivity with given
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chemical agents (Liew et al., 2011). However, increasing curing temperature fasten the setting
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time, due to an increased rate of chemical reaction that accelerates the hardening of geopolymer
mortar (Thakkar et al., 2014), (Hung et al., 2011; Wang and Cheng, 2003). Increasing
temperature of curing above 600˚C decreases setting times; beyond this temperature, setting
times is decreased extremely (Dimas et al., 2009), (Van Chanh et al., 2008). The curing time was
varied from 4 to 96 hours. It was found that the heat curing time shouldn’t exceed 24 hours; after
this time, curing time was not significant (Mishra et al., 2008), (Keshari et al., 2018), (Tempest
et al., 2009). However, the elevated temperatures are preferable in case precursors didn’t
undergo any thermal treatment. When the precursors were primarily treated thermally, then the
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paste can be cured at room temperature or a temperature degree < 100 ˚C. An increase of
temperature of heat treatment caused a decrease of Si/Al ratios in aluminosilicate gel, and long
curing at room temperature narrowed the range of distribution of the Si/Al ratios. Optimization
of curing time is mandatory, for example, fly ash activated by sodium silicate, 6 h heat curing is
The term ‘rest period’ is defined as the time from the end of casting to the start of hot curing.
The compressive strength for mixture with no rest day was 37.5 MPa, while only one rest day
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increased this value to 46.4 MPa (Lloyd and Rangan, 2010). The introduction of a rest day that is
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ambient curing for 24 hours prior to steam curing resulted in high compressive strengths of the
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order of 20%. The compressive strength of specimens increased with a rest period of one day or
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more after casting. The strength gain is up to 20 - 50 % compared to the blank specimens with no
rest period (Bakharev, 2005). Muhd Fadhil Nurruddin et al. reviewed different curing regimes
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(Nurruddin et al., 2018). Nuruddin et al. (Nuruddin et al., 2011) compared three curing regimes,
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and they found that external exposure resulted in the highest compressive strength. The effect of
different curing methods (with/without moisture and temperature control, associated with alkali
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activators was also investigated (De Rossi et al., 2020). Figure (13) shows the effect of these
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Fig. 13: EDS spectra of geopolymers with four curing methods (thermal conditions (TC), hydrothermal
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conditions (HC), water submerged conditions (SC) and usual conditions (UC)) and sodium silicate:
sodium hydroxide 1.5 at 28 days (De Rossi et al., 2020).
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Synthesis reaction and how it affects the final product of geopolymer occurs through four basic parallel
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steps: the dissolution of alumino-silicate in specified alkali activators (sodium or potassium hydroxide
and sodium or potassium silicate). The reactivity of precursors depends on of the solubility kinetics of
reactive compounds which itself depends on the pH and surface area (Shi, 2001), reorganization of free
ion clusters to form coagulated structures, polycondensation to form the hydrated products (Komnitsas
and Zaharaki, 2007), (Alonso and Palomo, 2001; Dimas et al., 2009), (Zuhua et al., 2009), and finally,
hardening of the whole system to yield a final solid polymer (Singh et al., n.d.). Table 2 shows the
variation in compressive strength according to variation in precursors types, activators, and curing
regimes.
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Table 2: Different mixes conditions and the compressive strength of the final products.
Precursors Activator Curing Max. compressive Ref.
strength (N/mm2)
Fly ash + aggregates NaOH+ Heat 61.33 (Patankar et al.,
Na2SiO3 2013)
Fly ash Heat 60 (Kani and
Allahverdi, 2011)
Fly ash+ aggregates Hot gunny 22.7 (Nuruddin et al.,
+sucrose Ambient 27.3 2011)
External 50.9
of
exposure
Fly ash + aggregates Heat 32 (Brahammaji and
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Muthyalu, 2015)
Fly ash + aggregates n.a. 39.6 (Akbari et al.,
+ sand
Fly ash + kaolinite +
GGBS + aggregates
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Fly ash + GGBS + Ambient 80.5 (Krishnan et al.,
aggregates 2014)
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2014)
Fly ash + aggregates Ambient 30 (Bhikshma et al.,
2012)
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2.5. Properties
Geopolymers gain strength rapidly (Klabprasit et al., 2008) also enjoying high compressive
strength, low drying shrinkage, little creep (Hardjito et al., 2005), and good resistance to acid
(Thokchom et al., 2010), The references also discussed the mechanism of geopolymer resistance
toward sulfuric and nitric acids. The weight loss due to the exposure is only 0.5% compared to
concrete when immersed in 3% sulfuric acid (JAAFAR, 2014) and chemical attack (Lloyd and
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Rangan, 2010), (Hardjito et al., 2003). They studied the weight losses, decrease in compressive
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strength, change in microstructure, and hydration products, using XRD, FTIR, SEM techniques.
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They concluded that the weight loss was <3% after exposure to two acids for 24 weeks and no
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noticeable change in color. The loss in compressive strength was up to 70% in case of exposure
to both of acids for a long time. The mechanism of corrosion was mainly due to ion exchange
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and ejection of (Al) in tetrahedral sheets. The superior resistance of geopolymers to acid attack
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was attributed to that the hydration process resulting new aluminum oxide silicates and calcium
magnesium. Also, the concentration of the alkali activators strengthens the geopolymer
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resistance toward acids [124-134]. The performance of the geopolymer was much better than
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OPC, and the main loss in weight was due to the de-polymerization of alumino-silicates under
acidic medium. The best results obtained in case of curing at elevated temperature or/and using
NaOH as an activator.
It was also shown that the structural performance of geopolymer beams and columns similar to
that of OPC concrete (Sumajouw et al., 2007), (Sarker, 2009). Geopolymer has higher bond
strength than OPC concrete at the same test parameter (Sarker, 2010). Even the geopolymer
concrete withstand fatigue load (1332 cycles) higher than ordinary concrete (1151 cycles)
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(Deivabalan and Saravanan, 2015). The freeze-thaw properties of geopolymer were also
discussed in the literature. It was found that after recording 180 cycles, the compressive strength
and the mass losses were 5& 1%, respectively (Abdulkareem et al., 2014). Shrinkage <0.1% was
also recorded (Banah, 2014; Wallah, 2010). Finally, promising results for workability was
Recent studies stated that adding nanoparticles improve the mechanical properties of the
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geopolymer matrix (Rashad, 2019). They investigated the effect of adding additives like steel
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and polypropylene fiber (Barnard, 2014), titanium dioxide (Yang et al., 2015), nano-silica, and
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nano alumina (Nazari and Sanjayan, 2015; Phoo-ngernkham et al., 2014; Riahi and Nazari,
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2012) and other additives to geopolymers (Table 3). These nanoparticles act as nanofillers,
reduce the water, and increase the compressive strength. For example, adding TiO2 (5%)
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improves the mechanical properties of geopolymers (Duan et al., 2016). And even when this
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Aponte et al., 2017). Introducing SiO2 (<3%) improves the mechanical properties; this was
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attributed to its amorphousity and its participation during geopolymerization process (Assaedi et
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al., 2016) even at a very low weight percentage (1%), it can improve the strength and density
(Singh et al., 2018). Another candidate was carbon nanotubes (CNTS). The results showed that
adding only 0.5% of CNTS during geopolymer synthesis improved the flexural- strength and
toughness (Saafi et al., 2013), and in the case of adding 0.4% of CNTS, the compactness
increased (Khater and El Gawaad, 2016). Saafi et al. investigated the effect of graphene oxide on
geopolymers characteristics; they concluded that the porosity decreased and the strength
increased where these nanoparticles chemically bond the geopolymer matrix (Saafi et al., 2015).
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The best results were in case of adding SiO2 nanoparticles because it acts as the main
Even they synthesized a nano-geopolymer by reducing the size of the fly ash precursor to less
than 100 nm and curing at 70˚C (Al Bakri et al., 2013b). However, adding more than 3% of
nano-kaolin is not preferable, where at a higher percentage, the nanoparticles agglomerated and
the resulting negative effect (Hassaan et al., 2015). In contrary to Dufková and Kovačič, who
studied the effect of SiO2 nanotubes, carbon nanoparticle, and nanofiber on geopolymer
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composite, the results were not good, they attributed this to the low adhesion of these
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nanoparticles to the matrix and also the mechanism is still unclear (DUFKOVÁ and KOVAČIČ,
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n.d.). The dolomite-concrete powder was used to enhance the mechanical properties of a
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geopolymer (Ouda and Gharieb, 2020). There was a particular focus on the effect of different
fiber on the mechanical properties of geopolymers (Al-Majidi et al., 2017; Bhutta et al., 2017;
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Herbert Sinduja et al., n.d.; Ranjbar and Zhang, 2020; Sukontasukkul et al., 2018).
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deformation
Mineral additives Mineral additives can compensate the (Bondar et al., 2010)
shortage of the geopolymer main
oxides
Wollastonite The optimum value for maximum (Silva and Thaumaturgo,
toughness was 2% 2003)
Vermiculite Enhancing fire resistance (Temuujin et al., 2012)
Natural Bamboo fiber Production of green material of (Ribeiro et al., n.d.)
construction
Zircon Mineral Adding <10g/100g of metakaolin (Zawrah et al., 2018)
improve the mechanical properties of
the final product
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Slag The optimum value for improving (Li and Liu, 2007)
mechanical properties was 4%
Ammonium molybdate ammonium molybdate governs the
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(Vidal et al., 2015)
polycondensation process
Nano sand 2.5% of nano sand increase (Zawrah et al., 2020)
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polymerization and enhance the
properties of the final product
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Silica fume The silica fume increase the reactivity (Lee et al., 2016)
of the fly ash- slag based geopolymer
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sulfate
Portland cement Additional C–S–H & C–A–S–H (Pangdaeng et al., 2014)
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Reduction in CO2 emissions has been measured up to 0.73 ton CO2/ton of OPC replaced by
geopolymer (Dai et al., 2013). Additionally, the disposal of some precursors such as fly ash, slag,
and other industrial byproducts require large quantities of area and energy, so managing of these
wastes for production of green geopolymers considered an added value and minimizes the need
for clay and limestone in construction building manufacturing (reticulate Blanco, n.d.). Finally,
a reduction in the cost from 12 up to 30% can be achieved in case of replacement of OPC by
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For sustainability, construction building material industry needs to explore green binder instead
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of OPC, the need for industrial wastes and low-cost materials-based geopolymer reduce global
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warming (Lloyd and Rangan, 2010) and get rid of a massive amount of wastes.
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In the past, OPC was blended with geopolymer cement to merge the merits of geopolymer like
fast hardening (4 h) compared to OPC which needs several days and the low cost of OPC,
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especially in the military and industrial buildings (Husbands et al., 1994; Malone et al., 1985).
na
In the present future, there might be wide applications for geopolymer in construction building
material (Aleem and Arumairaj, 2012b). Gourley and Johnson have reported a list of products
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that geopolymer has been involved for, included sewer pipes, railway sleepers, and wall panels
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(Gourley and Johnson, 2005), paving material (Davidovits, 2002; van Deventer et al., 2013),
electrical fuses (Davidovits, 2002) (Fig. 14). Wilkinson et al. reviewed the application of
geopolymer in road applications; they draw attention to the importance of putting standards
specific to the production of geopolymers (Wilkinson et al., 2015). Finally, geopolymers have
the ability to stabilize some hazardous materials that cannot be immobilized in OPC (De Weerdt,
2011) like lead (Li et al., 2015; Pereira et al., 2009; Xia et al., 2019) and boron (Ekaputri et al.,
Journal Pre-proof
2010). Also, they can solidify some radioactive wastes (Shi and Fernández-Jiménez, 2006;
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Fig. 14: Paver block (Vaz et al., 2012), electrical fuses (Davidovits, 2002), extruded kerb made (Glasby et
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al., 2015) of geopolymers.
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The geopolymer was even recycled in ordinary concrete; it was reported that replacing up to
20% of concrete aggregate with recycled geopolymers results in a small reduction in flexural
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strength and modulus of elasticity and a moderate reduction in compressive strength (Mesgari et
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al., 2020). The environmental impact of fly ash-based geopolymer was assessed, one of the
major findings of the study is that the most negative impact raised from using the alkaline
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activator. Also, sustainability raised from good environmental impacts and cost reduction
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A lot of studies on geopolymers have been published during the past years, but much work still
needed. However, there is some limitation for the sustainability of geopolymers like
efflorescence (formation of white salts on the surface when contact with humid air. These salts
deposit rises from using alkaline solution during geopolymerization (Ribeiro et al., n.d.).
1. Searching for new industrial wastes based on silica and alumina and investigate similar
pozzolanic materials.
5. Searching for new nanoparticles and additives is an important research area since
nanoparticles may solve challenges like efflorescence, cost, and environmental issues,
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etc.
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6. Contribute to solving climate change problems.
5. Conclusion
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This paper summarizes the research findings related to the production of geopolymers. The
current knowledge shows that the precursors' type, precursors/alkaline ratio, mixing mechanism,
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and curing- time and temperature are essentials for achieving the optimum mechanical properties
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hydroxides and silicates. The molarity of the alkaline solution plays different important roles in
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the synthesis process, the optimum molarity in numerous studies was 12 M of NaOH. Some
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geopolymers can be cured at room temperature, but it preferable to increase the temperature (>
60˚C), especially when the precursor didn’t receive any heat treatment. The maximum curing
time was 24 h; behind this period, the curing will not be sufficient. Although recent studies in
the application of nanoparticles in the geopolymer matrix were reviewed, however, there is still a
gap to transfer such technology from the laboratory to the large scale. It can be concluded that
the activator is the governing factor in geoploymerzation process and cost. Searching for new
activators is mendatory for lowering the cost at the large scale production and the sustainability.
Journal Pre-proof
through nano-sized additives will yield good impact in reducing the cost and enhancing the
mechanical properties. The hope is that this paper will help researchers for searching how to
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☒ The authors declare that they have no known competing financial interests or personal relationships
that could have appeared to influence the work reported in this paper.
☐The authors declare the following financial interests/personal relationships which may be considered as
potential competing interests:
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