1 s2.0 S2352710222001176 Main
1 s2.0 S2352710222001176 Main
1 s2.0 S2352710222001176 Main
A R T I C L E I N F O A B S T R A C T
Keywords: Geopolymers have been recognised as a viable replacement to ordinary Portland cement (OPC),
Geopolymer concrete providing a cleaner solution since it can significantly reduce greenhouse gas emissions as well as
Mechanical properties accomplishing effective waste recycling. Construction and demolition waste (CDW) has been
Construction and demolition waste (CDW) recently identified as raw materials for geopolymers due to its availability and high contents of
Mix design silica and alumina. This paper aimed at reviewing the current state-of-the-art on the geopolymer
Sodium silicate
paste, mortar, and concrete production and their properties, with special attention paid to geo
Life cycle assessment
polymers incorporating CDWs. The review covers brief assessment of using CDWs in concrete, the
mix design of geopolymer mixtures in addition to identification of the main factors influencing
the performance of geopolymer containing CDW. The most recent data related to the mechanical
and durability properties of CDW-based geopolymers are presented, while the cost and envi
ronmental impacts of using recycled materials in producing geopolymer concretes are also dis
cussed. Geopolymer concretes have a vast range of possible applications, however, there are still
several barriers facing commercialisation of geopolymers in construction industry. The review
indicated that it is possible to produce geopolymer concretes from CDW-based materials with
properties comparable to OPC-based ones; however, the selection of proper material composition
should be carefully considered, especially under normal curing conditions.
1. Introduction
Concrete is the most used material in the construction sector, reaching approximately 30 billion tonnes of annual global con
sumption levels [1], depleting large quantities of ordinary Portland cement (OPC), which is the fundamental binder used to produce
conventional concrete. However, the production of cement is associated with serious harmful environmental issues such as intensive
consumption of natural resources and greenhouse gas emissions. 1.5 tons of raw materials are approximately needed to produce one
ton of cement, which directly generatesaround 0.55 tons of CO2, while the combustion of fuels produces almost 0.4 tons of CO2,
releasing a total of 0.8–1.0 tons of CO2 emissions [2]. According to Madlool et al. [3], the cement industry is also linked to consuming a
significant amount of fossil fuels, representing proximately 12–15% of industrial energy. Globally, it is estimated that the manufacture
of OPC generates around 1.35 billion tons of greenhouse gases every year, representing 6–9% of the global greenhouse gas emissions
[4], which is mainly caused due to the combustion of fuel in the furnace, de-carbonation of limestone, and consumption of electrical
* Corresponding author.
E-mail address: m.m.a.alhawat@bradford.ac.uk (M. Alhawat).
https://doi.org/10.1016/j.jobe.2022.104104
Received 16 December 2021; Received in revised form 12 January 2022; Accepted 22 January 2022
Available online 28 January 2022
2352-7102/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
energy. Several chemical processes occur during the calcination of calcium carbonate; however, Equation (1), below, describes the
main reactions that occur during the calcination of limestone and aluminosilicate materials [5,6].
Over the past three decades, there has been a growing awareness of the environmental concerns associated with the manufacturing
of ordinary concrete, which has driven the researchers and cement industry to search for other methods to produce green sustainable
materials. More recently, the World Green Building Council (WGBC) (2019) has published the strategies and guidelines for designing
sustainable buildings and infrastructures with a plan to reach 40% lower carbon footprints by 2030, while the target is to attain zero
CO2 emissions by 2050. The main suggested actions are associated with using alternative fuels, capturing carbon dioxide and
enhancing energy efficiency inside the furnace, replacing cement with nanoparticles and developing low-impact green concrete
products and technology. Accordingly, geopolymers, which belong to the last option, have appeared as one of the most successful
alternatives to OPC-based binders/materials. This is not only related to geopolymers’ favourable environmental impact of reducing the
energy consumption [7], and using waste materials, but also due to their superior mechanical and durability characteristics accom
panied by the high potential of cost reduction [8], along with the excellent resistance against acids and high temperature [9,10]. Using
geopolymers as a OPC substitute can also reduce the overall CO2 footprint compared to traditional concrete. However, the rate of
reduced emissions is widely varied as stated in previous assessments, ranging from 9% [11], to 26–45% [12], and reaching up to
around 80% [13]. These huge differences are mainly associated with some key factors including transportation emissions, which are
mainly linked to the availability and proximity of raw materials, concrete mixture compositions, activator type/quantity needed and
production method used, and high-temperature curing.
Geopolymers are referred to the family of alkali-activated materials, and can be produced by polymerizing different types of
aluminosilicate precursors through activation processes using highly alkaline liquids and soluble silicates [14,15]. The precursors can
originate from natural sources (e.g., clay and kaolinite) [16] or from by-products such as fly ash and ground granulated blast-furnace
slag (GGFBS), which are no longer classified as waste materials due to their widespread and successful utilisation in the concrete
industry as separate pozzolanic materials. These precursors can be singly used or mixed with each other. Hence, increasing attention is
being paid to seeking other resources that can be successfully used in geopolymers to mitigate the huge demand for by-products.
On the other hand, there is an urgent need to find novel approaches to reuse the massive quantities of waste materials, resulting
from construction and demolition practices. It is reported that more than 800 million tons of CDW are annually generated in EU
countries [17]. Literature studies have explored the feasibility of incorporating CDW in producing sustainable concretes with satis
factory mechanical and durability performance [18–22]. However, the majority of these studies have mainly concentrated on utilising
CDWs as a replacement to natural aggregates.
Recycling and re-using CDWs as geopolymer sources can offer a sustainable solution for reducing their ecological impact and
decreasing OPC demand. More recent studies [23–26] showed an excellent opportunity for CDWs to be used as aluminosilicate source
materials for geopolymer binders. This is especially important considering the massive quantities of fine silt particles that are rich in
crystalline aluminosilicates, resulting from demolishing of structures. However, the target of developing a high-sustainability
CDW-based geopolymers with sufficient mechanical, fresh, and structural properties has not been completely investigated. Limit
edly available research in the literature has only focused on quantifying the materials utilised for producing paste and mortar as well as
testing their mechanical and microstructural properties [27,28], whilst no significant work has been found on CDW-based geopolymer
concrete. Based on the available findings, it is possible to attain sufficient mechanical properties by using CDW-based constituents
solely, while better performance can be achieved by combining CDWs with low quantities of OPC (up to 30%), reaching up to 102 MPa
compressive strength at 28 days [29]. However, the most successful findings were achieved under high-temperature curing (higher
than 60 ◦ C) [30–32], since it can enhance the precursors’ reactivity and facilitate the geopolymerization process [33], limiting their
environmental benefits and in-situ applications.
This paper reviews the current studies related to geopolymer pastes, mortars and concretes, with particular emphasis on CDW-
based ones. The paper initially presents a brief assessment of the use of CDW in concrete, with more attention on incorporating
CDW-based materials in geopolymers as fine/coarse aggregates and precursors, followed by the principles of geopolymerization
process and the mixture design of geopolymers in addition to identification of the main factors influencing the performance of CDW-
based geopolymers. Then, the most recent data related to the fresh, mechanical and durability properties of CDW-based geopolymers
are presented along with the life cycle assessment of using waste materials in geopolymers in terms of cost and environmental aspects.
Finally, the barriers and challenges to industry adoption are highlighted with a view on the way forward for future research.
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principle of all such techniques, in fact, is mainly based on either, removing the weak layer of adhered mortar or modifying and
strengthening the old mortar. Despite the efficiency of these techniques in improving the quality of recycled aggregates, some barriers,
especially those related to economic reasons, are still preventing the widespread reuse to be a realistic option. Many countries are still
commercialising since adequate taxes accounting for the environmental impact of its extraction are not implemented. Furthermore,
some recycling plants are not highly motivated to improve the quality of recycled aggregates [47]. Several national existing speci
fications and standards (e.g., RILEM, 1994; NEN-5905, 2010; WBTC, 2002; EHE-08 DIN D, 2002) allow the use of recycled aggregates
in producing concrete [48–52]. While some countries like Spain and China, only allow limited of recycled aggregates and require
concretes to be produced with at least 90% of natural aggregates with attached mortars [49,50], other countries such as the
Netherlands and Germany include the use of mixed recycled aggregates for producing concretes in their specifications with variable
proportions of crushed concrete, bricks, ceramics and asphalt [51,52]. In Spain, Annex 15 of the Code for Structural Concrete (EHE-08)
allows the use of recycled aggregates in concrete as long as the water absorption value does not exceed 7%. In fact, the main concrete
codes of practice, for example, Eurocode 2 (2008) and ACI-318 (2014) did not include any clause for structural members with recycled
aggregate concrete [53,54]. It should also be considered that the environmental and economic benefits of utilising recycled aggregates
are greatly affected by the location of demolition sites and the cost of transportation [55].
On the other hand, some other studies highlighted the improper properties caused by the low quality of fine waste grains, which are
mainly correlated to their low bulk density and specific gravity in addition to the higher porosity, abrasion loss and water absorption,
subsequently leading to low mechanical and durability properties [56,57]. However, the results obtained from other studies suggested
that up to 50% weight replacement of natural sand by CDW-based fine particles might have insignificant effects on the concrete
characteristics [58]. On the other hand, the use of CDW constituents without any treatment as a substitution for either fine or coarse
aggregates is not advisable, and it can highly negatively affect the properties of concrete due to expected high increments in porosity
and water absorption accompanied by a density drop [59,60]. According to Sata and Chindaprasirt [61], CDWs can be utilised as
aggregates in geopolymer concretes with possibly enhanced characteristics such as thermal insulation and low density; however, a
slight reduction in durability and mechanical properties would be expected, similar to the case of conventional concrete.
Recently, the effects of CDW-based fine particles used in geopolymer mortars as an alternative to natural sand have been inves
tigated [62]. The findings illustrated that the partial use of such aggregates could lead to even higher flexural and compressive
strengths compared to natural sand since a denser geopolymer is formed at paste-aggregate interfaces. However, the full inclusion of
CDW-based aggregates as a substitution to natural sand in geopolymer mixtures should be avoided, especially under aggressive
conditions due to highly increased absorption capacity of CDW-based mixtures. Therefore, it is recommended not to exceed 25% of
recycled fine aggregate in concrete mixtures as a replacement to natural sand to obtain mechanical properties comparable to those
with natural aggregates [63]. During the crushing process, a considerable amount of fine powder is generated, accounting for
approximately 15–20% of total waste concrete [64]. Studies conducted on the use of this powder as a partial replacement to cement are
limited in number. Kim and Choi [65] found that adding concrete waste powders to geopolymer mortar had a significant detrimental
impact on the fluidity and compressive strength, and it is preferable not to exceed 15% as a replacement rate. In a recent study, Ma
et al. [66] highlighted that using up to 30% CDW powder in conventional concrete instead of OPC can facilitate the hydration process
and minimise the permeability and porosity, while the higher ratios could lead to significantly negative effects, especially on properties
like frost resistance and chloride ion permeability. Schoon et al. [67] highlighted the viability of partially employing fine powder from
recycled concrete as an alternative source for producing Portland cement clinker. The waste hydrated cement obtained from the
separation of fine recycled aggregate would be of significant importance in the chain of the cement industry. This is mainly attributed
to the presence of inorganic substances forming after the drying process, which have almost similar chemical compositions found in the
raw clinker and its use in replacing natural quarried minerals, reducing the consumption of raw materials. However, the quantity of
waste hydrated cement used as a raw powder in producing Portland cement clinker is limited by the chemical composition of waste,
particularly the CaO/SiO2 ratio [68]. Nevertheless, these approaches have not addressed the problem of CO2 emissions in a funda
mental way, and they still represent significant environmental risks due to the low potential rate of use of CDW-based powders in
conventional concrete. Such powder is mostly composed of hydrated cement rubble, unhydrated cement particles, fine powder of
aggregates/bricks, which can meet the fundamental characteristics of geopolymer source materials considering their aluminosilicate
compositions.
3. Geopolymerization process
Geopolymers can be considered as alkali-activated binders or amorphous alkali aluminosilicates [19]. During the geo
polymerization process, inorganic compounds are generated after several complex chemical reactions between the aluminosilicate
oxides in highly alkaline environments to form three-dimensional polymeric Si–O–Al–O chains as the main alkaline aluminosilicate
gel. Several investigations have been made on the chemical reactions of geopolymers [69–71]. Geopolymerization mechanism is
highly dependent on the nature of alkaline activator as well as the chemical composition of precursors. Due to numerous components
available in the liquid phase, all reactions take place at the same time and affect each other [72]. Thus, geopolymerization mechanism
can be stated to be more complex than OPC hydration. According to Davidovits [69], geopolymerization consists mostly of four phases.
The alkaline activator firstly breaks Al–O and Si–O bonds in the aluminosilicate precursors, releasing Al–O and Si–O tetrahedral
monomers (dissolution), before being diffused in the reaction system (diffusion). According to the concept of chemical equilibrium, the
concentrations of silicon and aluminum drop on the particle surface due to diffusion, while the dissolving process proceeds. In the next
stage (polycondensation), Al–O and Si–O tetrahedral units are converted into amorphous -Si-O-Al-O-structures or even zeolite crystals
during the polymerization. Finally, the dehydration process takes place, resulting in a hardened geopolymer with mechanical strength
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Fig. 1. Final gels formed based on the chemical compositions of the precursors [75].
(hardening). It should be noted that the geopolymerization process for geopolymer materials sourced from varying raw materials are
not identical, although they fundamentally follow the aforementioned reaction sequence. Similar geopolymerization mechanisms
were suggested by De Silva et al. [70], with three main stages. The initial stage, termed as the dissolution stage, which involves
dissolving alumina and silicate in the precursors, forming SiO4 and AlO4. Therefore, only precursors with aluminosilicate content can
be used to produce geopolymer [70]. In the second stage (agglomeration), the condensation process starts when the dissolved in
gredients react with each other as well as with alkali cations (K+ or Na+). Geopolymerization occurs in the last stage by
poly-condensation of such dissolved ingredients, consequently forming a three-dimensional aluminosilicate (Si–O–Al–O) structure in
an amorphous to semi-crystalline form as given in Equations (2) and (3), below [72,73].
Unlike the model of Davidovits, the conceptual model presented by Glukhovsky [71] divided geopolymerization processes into
deconstruction, gels formation, poly-condensation, and crystallization steps to eventually produce a 3D network structure of geo
polymer. The main difference compared to the model of Davidovits seems to be the polycondensation process that is separated into two
steps, namely gelation, and reconstitution. Gelation requires de-hydration to generate oligomeric gels when aluminosilicates are
saturated, whilst reconstitution covers the rearranging of the oligomeric gels. It is worth noting that water plays no role in geo
polymerization reactions, and it simply improves the workability of the mixtures, in contrast to the hydration process of OPC-based
concrete [69,72].
As exhibited in Fig. 1, the formation of the final gel is highly dependent on the nature of aluminosilicates as well as the activator
used. Calcium aluminosilicate hydrate (C-A-S-H) gel is the main product formed in the presence of precursors with high-calcium
content such as GGBFS and class C fly ash, which is similar to calcium silicate hydrate (C–S–H) gel formed through the hydration
of OPC. However, amorphous aluminosilicate gels (N,K-A-S-H) are formed as a result of the geopolymerization of precursors with low
CaO/SiO2 ratios, such as clay and class F fly ash. According to Garcia-Lodeiro et al. [74], the stability of N-A-S-H structure is heavily
affected by pH alkalinity. At low alkalinity, sodium is partially replaced by calcium, resulting in the formation of C-(N)-A-S-H gel.
When the pH exceeds 12, the presence of CaO destabilises the N-A-S-H, resulting in the formation of the C-A-S-H type phase. The nature
of the alkaline solution can also affect the structure of the final gel, since different atoms of Al and Si can be found in the hydroxide or
silicate used [75]. Although potassium hydroxide provides higher alkalinity, sodium hydroxide has shown a higher capacity to dissolve
silicate and aluminate species [76,77].
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Fig. 2. The target strength mix design method for geopolymer mixture [84].
of geopolymer concrete to cover densities, air contents, specific gravities of components, workability and compressive strength.
However, the main challenge that emerged with this process was the determination of the alkaline activator to binder ratio. Pavithra
et al. [81] suggested a relationship between water-binder ratio (W/B) and compressive strength by fixing the activator content,
allowing the design of mixtures to be more flexible in terms of activator content and desired strength, while the aggregate content was
calculated by using the grading curve of combined aggregates. Moreover, Li et al. [82] suggested guidelines for selecting the pro
portions of geopolymer mixtures with a strength of 40–80 MPa. In their technique, the principles of compact packing of aggregates and
Taguchi method were adopted. In concrete design, the main targets are mostly workability and compressive strength; hence, these
targets are used to determine the contents of precursors, activators, aggregates and water. In conventional concrete, the workability
and strength can be modified by water content (water-binder ratio [W/B]) and binder content (paste-aggregate ratio) [83]. Similarly,
the binder in the geopolymer system is formed as a result of alkaline activation reactions [84], and thus, the type, quantity, and
concentration of alkaline solution used need to be considered. In geopolymer concrete, alkaline solution is a costly component, and
from the economic point of view, the amount of alkaline solution should be minimised, while maintaining the desired workability and
strength [81]. The flow chart in Fig. 2 summarises the overall mixture design process for geopolymer concrete (GPC) as suggested by Li
et al. [84]. The alkaline activator-to-binder ratio (AL/B) can initially be selected, using the relationship between W/B and the desired
compressive strength described in ACI 211.1 [85] for conventional concrete. Similar to the W/B ratio in concrete, AL/B represents the
total mass of alkaline solutions to the mass of precursors; however, the compressive strength of geopolymer is often higher than that of
conventional concrete at the same AL/B ratio. Then, the amount of binder can be calculated according to one of three methods, namely
fixed water content, fixed binder content, and fixed paste content. The constant water content is governed by the aggregate size and
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Table 1
Chemical composition ranges for different aluminosilicate materials [7,24,25,31,96,99–107].
SiO2 53–70 23–42 57–70 70–75 35–47 38–65 26–40 45–61 16–25
Al2O3 11–20 4.0–10 10–18 1.0–2.5 15–20 24–50 5–17 32–52 2.9–5.1
CaO 0.5–11 20–31 2.9–8.7 8–12 20.96 0.7–5.2 34–54 0.02–0.1 60–66
Na2O 0.2–2.5 0.6–1.7 0.5–1.4 11–15 4.0–4.9 0.05–0.9 0.03–0.5 0.15–0.25 0.2–0.4
MgO 1.1–5.2 1.5–8.4 0.42–3.1 0.15–1 4.5–5.0 0.3–1.8 4.0–10.9 0.03–0.4 1.5–1.8
Mn2O3 0.05–0.15 0–0.1 0.06–0.2 0–0.1 0.03–0.1 0.0–0.7 0.3–0.6 0.0–0.1 0.3–0.45
Fe2O3 5.5–8.2 2.9–12 1.1–5.2 0.15–1 5.0–6.1 2.0–13 0.6–2.0 0.35–2.6 4.0–8.2
K2O 2–4.5.0 0.7–2.3 1.1–2.3 0.08–2 0.5–0.9 0.1–3.0 0.05–1.0 0.2–1.3 0.05–0.1
TiO2 0.8–1.1 0.2–0.3 0.8–1.5 0.07 1.0–1.9 0.5–2.0 0.3–0.6 0.8–2.0 0.2–0.3
Loss on ignition 0.4–2.0 0.7–8.2 1.6–2.1 0.2–1.2 0.25–1.5 0.03–7.7 0.02–2.05 0.5–2.4 0.5–2.0
Note: BW = bricks waste; CW = concrete waste, TW = tile waste; GW = glass waste; FA-C = class C fly ash; FA-F = class F fly ash; MK = metakaolin, OPC=Ordinary
Portland cement.
required workability based on ACI 211.1 standard [85] for cement-based concrete. According to Reddy et al. [86], 200 kg/m3 alkaline
solution can be sufficient to provide satisfactory workability for geopolymer mixtures. Moreover, the constant binder content is
typically selected based on available research and does not consider aggregate characteristics. For example, Junaid et al. [87] indicated
that 360–420 kg/m3 of fly ash (FA) content can be used to produce geopolymer with good strength (25–60 MPa), whilst Ferdous et al.
[78] suggested some relationships to select FA content according to AL/B and compressive strength. However, using different sources
of precursors materials can affect the findings, especially CDW-based materials, which require modification of binder content. The
quantity of aggregates can be determined based on the absolute volume method. Sing et al. [88] suggested a relationship between the
packing density of aggregates, binder content and compressive strength in geopolymer mortars, which might be applied for geo
polymer concrete. The packing fraction technique uses volumetric proportioning of fine and coarse aggregates based on optimising the
best particle gradation curve obtained. The principle of this approach is to choose a particle size distribution that can fill the gaps
between small and big particles with the paste, which, in turn, can improve the workability and compressive strength at early ages
[84–89]. Statistical modelling approaches such as the Taguchi technique might also be applied for designing geopolymer concretes,
considering the main parameters in geopolymers. The Taguchi technique employs a factorial design approach that needs the use of
orthogonal arrays of experimental designs with many variables. Orthogonal arrays are mainly used to minimise the uncontrollable
factors during design; thus such technique might be used to assess a single property by maximising the interaction of various factors
[90,91]. However, this approach is restricted to certain levels and cannot always be applied, and hence a large database is required in
order to develop this method.
It can be concluded that although some methods are suggested, further developments on these methods are still needed, consid
ering the variations of the materials used (e.g., CDW) and other influencing parameters. It should be noted that testing at the age of 28
days is not always ideal for determining the final properties of geopolymers due to the variations of the materials used. For instance,
the activated mixtures based on slag and metakaolin can reach their ultimate strength sooner than 28 days, whilst the fly ash based
mixtures continue developing strength even after the 28-day testing period [92].
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Fig. 3. Effect of inclusion of SCMs on the compressive strength of CDW-based geopolymers [25].
performance of mixed CDW-based components with different levels of replacement or even without any component separation to
simulate the realistic cases [27,98]. Geopolymers produced from waste bricks and ceramic powder exhibited much higher mechanical
characteristics in comparison to that containing only waste concrete, reaching compressive strength of 58 MPa after 7 days of heat
curing [31], however, recycled glass showed relatively low enhancement in strength [98]. The variations in the performance of
CDW-based geopolymers can be ascribed to the varying levels of chemical compositions of precursors, particularly silica, alumina,
calcium, iron and magnesium. The ranges of the chemical composition of aluminosilicate precursors (including CDW-based ones)
collected from different investigations [7,24,25,31,96,99–107] are presented in Table 1. It can be noted that the high quantity of SiO2
can be found in both bricks and tiles (50–70%) with less amount of Al2O3 (10–20%), compared to concrete waste with SiO2 range of
only 23–42% of and Al2O3 of 4–10% available in concrete waste. Therefore, the high contents of Al and Si ions can be easily stabilised
during the activation process and subsequently participate in forming Si–O–Al bonds [31]. On the other hand, only waste concrete
contains a sufficient quantity of CaO, while other CDWs (e.g., bricks and tiles) have only low ratios of calcium. The presence of the high
content of CaO in waste concrete is mostly linked to the drop of concrete strength as it consumes a large part of NaOH solution [94,
108]. Thus, balancing the main elements (i.e., SiO2, Na2O, Al2O3 and CaO) is crucial for the geopolymerization process to attain an
ideal geopolymer synthesis.
5.1.1.2. Addition of supplementary cementitious materials. Considering the chemical compositions of CDWs, additional sources of
precursors such as OPC [102,109], GGBFS [24], metakaolin and fly ash [110] can be incorporated to aid in producing denser and
stronger geopolymers. For instance, if bricks are used as a precursor, GGBFS can be recommended to be added to cover the CaO
shortage, while in the case of use of concrete waste, metakaolin or fly ash inclusion can nourish the results as they contain high
quantities of SiO. The activation process of CDW is exceedingly slow, resulting in decreased/no strength growth at early ages most
probably due to lower calcium concentration and crystalline form. Some relevant studies [111] reported that the use of waste bricks as
precursors did not exhibit any strength development at early ages, while the compressive strength was clearly improved when waste
bricks were combined with GGBFS as also reported by Rakihmova et al. [106] who suggested that bricks waste can be used in mixture
with GGBFS up to 60%. This can be justified since GGBFS acts as a source of calcium, providing substantial quantities of Ca2+, Si4+ and
Al3+ to be leached out during the activation process, resulting in a rapid enhancement in strength. In a recent study, Mahmoodi et al.
[25] investigated the influence of the most common types of SCMs (i.e., FA-C, FA-F, GGBFS and metakaolin [MK]) on the compressive
strength of geopolymer binders made from waste concrete and bricks under ambient conditions. CDW powder in the mixtures was
partially replaced by abovementioned SCMs (15%, 30% and 45%) and confirmed that the inclusion of varying percentages of SCMs
leads to a significant enhancement in the compressive strengths of all mixtures tested, compared to mixtures with no SCM substitution
(Fig. 3). However, the use of GGBFS (45%) showed an outstanding enhancement rate (almost 208%) at 28 days, whilst using the same
replacement level with MK, FA-C and FA-F led to 80%, 45% and 33% improvements in strength, respectively. This can be due to that
the balanced levels of Si/Al and Na/Si with sufficient OH− and Na+ contents may have provided an improved breakage of the bonds as
Si–O–Si, Al–O–Si, Al–O–Al, and Ca–O, which were available in waste concrete/bricks and GGBFS [112]. Therefore, further amorphous
C-A-S-H, C–S–H and N-A-S-H would be formed.
It is also stated that during the geopolymerization process, lower concentrations of alkaline activators are needed for calcium-rich
precursors. For instance, Krivenko and Kavalerova [113] found that activator concentration between 5 and 20% is needed to activate
the binder made with fly ash and metakaolin, while only 2–8% could be sufficient to activate GGBFS-based geopolymers that are rich in
calcium. Calcium found in GGBFS can adjust sodium aluminosilicate gel (N-A-S-H) by partially substituting sodium ions with calcium,
in turn, contributing to the formation of C-(N)-A-S-H gels. The latter can improve the stiffness of the geopolymer mixture, especially at
room temperature [114]. The presence of free calcium ions during geopolymerization may also accelerate the dissolution of
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Fig. 4. Effect of particle size of precursors on the compressive strength of geopolymers [31].
aluminosilicates, increasing the heat of hydration and subsequently, enhancing the strength development of geopolymers [115].
Adding calcium oxide in the form of calcium hydroxide into mixtures as an additive can also effectively enhance the durability and
strength of geopolymers as it can improve the low reactivity of aluminosilicates available in waste materials as well as accelerate the
setting process [116]. However, there is a general agreement that a material containing more than 20% CaO is not favourable for
synthesising geopolymers owing to its rapid setting.
It is important to note that the predominant products of geopolymers prepared from clay-originated CDWs such as red clay bricks,
hollow bricks and roof tiles are N-A-S-H gels with zeolite-like structures, whereas sodium silicate gels mainly forms in glass-based
geopolymers [98]. Similarly, the main product from high-calcium precursors (e.g., GGBFS) is the C-A-S-H gels, which are similar to
that formed during the hydration of OPC (C–S–H). However, using low-calcium precursors such as calcined clays and FA-F mainly
results in the formation of amorphous N-A-S-H gels in 3D structures [25,75].
5.1.1.3. Fineness of particles. Besides the nature of precursors, the fineness of its particles plays a crucial role in determining the
characteristics of geopolymers. Finer particles of precursors could offer higher reactivity and stronger geopolymerization, which, in
turn, helps in producing stronger paste with a denser microstructure. This is mainly associated with the higher specific surface area
achieved in finer source materials, accelerating the reaction rate since the process of dissolution occurs faster, leading to a shorter
setting time and earlier development of strength. However, the improvements in mechanical and durability performances can only be
obtained by the balance between higher water requirement and fineness of source materials. As stated by Komnitsas [31], the
compressive strength of geopolymers can be substantially improved when the sizes of CDW-based particles are lower than 150 μm and
D50 is less than 15 μm. As exhibited in Fig. 4, the compressive strength of tile-based geopolymers activated by 10M-NaOH is increased
by more than 50% when the particle size decreased from 477 μm to 140 μm [31]. Similar observations were reported on samples
prepared with bricks, when the particle size reduced to from 350 μm to 140 μm, the compressive strength reached around 35 MPa. The
strength of geopolymers made from waste concrete was doubled when the finer particles (190 μm) were used instead of coarser ones
(400 μm). According to Hue et al. [107], only particles that are smaller than 125 μm can be alkali activated due to their higher
reactivity, whilst others [24,117,118] highly recommended that the particle size of CDW-based ingredients should be finer than 75 μm
to be used as precursors.
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
Fig. 5. Ternary diagram for the major oxides found in silica-rich waste source materials [132].
Fig. 6. Relationship between the NaOH concentration and compressive strength of geopolymers.
release aluminate and silicate monomers [124]. The use of alkaline activator solutions is considered one of the main practical limi
tations of geopolymers due to their high cost and carbon footprint associated with their production process, especially in the case of
sodium silicate [125]. Notably, the production of sodium silicate requires significant energy for melting sodium carbonate with silica
sand in the furnace at temperatures ranging from 1400 to 1500 ◦ C [126]. To enhance the commercial viability of geopolymers, it is
critical to minimise the costs associated with the production of activators while retaining their environmental friendliness and per
formance. More recently, alternative activator solutions have been synthesised from silica-rich waste materials including bottom ash
[127], rice husk ash [126], glass waste [128] and precipitated silica [129]. The silica extracted from such sources and dissolved in
alkaline solutions showed the possibility of reducing footprint emissions by up to about 50% compared to those generated from the
commercial ones [130,131]. However, the performance of such activators can vary widely based on some key factors, including the
amorphous silica content, extraction method and particle size. To aid in understanding the chemical composition of diverse silica-rich
wastes, Alnahhal et al. [132] developed a ternary diagram to illustrate the main oxides of various silica-rich wastes utilised in the
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Fig. 7. Influence of sodium silicate-to-sodium hydroxide ratio on the compressive strength of CDW-based geopolymers.
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
Fig. 8. Effect of SiO2/Al2O3 and Na2O/SiO2 ratios on the flowability of CDW-based geopolymers [101].
conducted on compressive strength of CDW-based geopolymer [107,122,137] indicated that the optimum ratio of Na2SiO3/NaOH
ratio would be in the range of 1.0–2.0 as illustrated in Fig. 7.
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
Fig. 10. Ion concentration of Si4+ versus dissolution time for CDW-based geopolymers at varying NaOH molarities [107].
setting time [162]. Faster setting of geopolymers incorporated with GGBFS and MK is also related to the virtual characteristics such as
the size and shape of the particles. In fact, the grains of MK and GGBFS mostly have finer particles and more angular shapes compared
to those extracted from CDWs. Therefore, it is recommended to use these calcium-rich products in producing CDW-based geopolymers
to accelerate the delayed setting, especially under ambient temperatures. However, the use of high contents of GGBFS in the mixture
can significantly reduce the setting time, especially over 50%, causing difficulties in the handling of the mixtures [163]. The disso
lution of CDW-based geopolymers is greatly influenced by the variations in alkaline molarity. Huo et al. [107] found that the pre
cipitation of Si4+ in geopolymers produced from concrete waste accelerated with the higher concentrations of NaOH. As it can be seen
from Fig. 10, the average participation level of Si4+ ions for the molarities of 10, 14 and 18 M was higher than 130 mg/l, which, in fact,
was considerably higher than that reported for 6 M. The low concentration of NaOH solution (6 M) was unsufficient for dissolving the
silicate and aluminate species in CDWs, hindering the rate of geopolymerization reactions. By increasing the concentration of alkaline
solution, more OH− ions come into contact with the surface of CDW-based particles, increasing the rate of dissolution of the Si–Al
phase and the concentration of Al4+ and Si3+ in the liquid phase, which in turn collide with each other to produce aluminosilicate gels.
However, the highest concentration (18 M) did not lead to better results, which is attributed to the delay in the mobility of ions, caused
due thickening of alkaline activator, preventing further ions from leaching out [164]. Thus, it can be stated that using either low
concentration (6 M) or high concentration (18 M) of alkaline solution is not favourable for hydrolyzing and precipitating Si4+ ions from
the solid aluminosilicate precursors. The findings also indicated that the precipitation of Si4+ in CDW-based geopolymers reached the
maximum after approximately 10 min for all NaOH concentrations used, while it tended to be stable after around 20 min for all NaOH
concentrations.
In terms of rheology, the aluminosilicate precursor has also a significant influence on the temporal development of yield stress and
plastic viscosity. Rovnaník and Rakhimov [116] found that the geopolymers made with brick powder exhibited the lowest rheological
performances in terms of both yield stress and plastic viscosity, while the use of MK caused a gradual increase in the yield stress. This
can be attributed to the higher reactivity of MK since it is mainly composed of amorphous deformed aluminium structure; hence,
allowing it to be quickly dissolved and instantaneous gelation of aluminosilicate oligomers. According to Kashani et al. [165], alkali
hydroxides produce a substantial rise in the yield stress of an alkali-activated paste, whilst sodium silicate causes a reduction in the
yield stress because of the deflocculating and plasticizing effects of silicate ions. The temporal development of yield stress and plastic
viscosity are significantly affected by the type of precursors used. Using large quantities of CDW-based powders in geopolymer
mixtures caused almost negligible changes in the viscosity, leading to more delay in the yield stress due to reduced presence of reactive
amorphous phases [166].
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temperature ranging between 400 and 800 ◦ C as reported in previous studies [31,168]. As can be noted, there is a gradual decrease in
the compressive strength of all tested samples with the increase in temperature. The reduction due to increased levels of temperature is
mainly attributed to increased porosity and shrinkage of the mixture accompanied by the weight loss, causing the reorganisation of
Si–Al bonds, and consequently leading to the development of microcracks [169]. Thermal instability in geopolymers is influenced by
the source of CDW-based materials [170]. As can be also observed from Fig. 11, the geopolymers made by bricks showed high
resistance to decomposition compared to those made by concrete and tiles, which is likely associated with the formation of extra
crystalline phases under heating due to greater amount of Al2O3 content in the bricks.
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
Fig. 12. Acid resistance of geopolymer mortar in comparison with cement mortars [171].
functional aspects of bricks-based geopolymer activated by a mixture of sodium hydroxide and sodium silicate were assessed. The
environmental impact was examined by analysing carbon dioxide emissions and energy consumption associated with the geopolymer
production. The combined environmental and functional aspects were expressed in terms of the energy consumption efficiency and
carbon dioxide emission efficiency index per one MPa. As depicted in Fig. 13, the findings indicated that the inclusion of 70% of waste
bricks in geopolymer provided compatible strength to OPC paste, while 45% on energy and 72% on greenhouse gas emissions can be
saved. This is mainly owing to using low quantities of sodium hydroxide and sodium silicate as their detrimental impacts on the
environment were more significant, as shown in Table 2. Higher energy consumptions and CO2 footprints, 63% and 81%, respectively,
could be saved, but lower mechanical performances were obtained.
Lloyd and Rangan [173] stated that even after accounting for the cost of the alkaline solution required to produce the geopolymer
binder, geopolymer concrete is predicted to be 10–30% cheaper than similar concrete prepared from OPC. Accordingly, geopolymers
would be expected to be more affordable when CDW-based materials are used as precursors. In a recent study [174], a comprehensive
cost analysis on the manufacturing of geopolymer bricks was calculated by using various formulations of bricks (GWB1-5) made by
waste bricks and GGBFS, and compared with the geopolymers made by clay (GC) and fired bricks (FB) to determine the economic
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
Table 2
Energy consumption and CO2 emissions for the CDW-based components [172].
Fig. 14. The cost of producing one metric tonne of brick and relative compressive strength of geopolymer [174].
viability of producing geopolymers at the industrial scale. The cost of producing a metric tonne of bricks and all manufacturing stages
of geopolymer bricks were calculated using the brickworks model from the French market. The findings shown in Fig. 14 indicate that
geopolymer bricks manufactured from waste bricks could achieve double compressive strength with the same manufacturing cost used
for the traditional bricks. They also confirmed that the sodium silicate used in producing a metric tonne of geopolymer is the most
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
- The variations of CDW properties, as depicted in Table 3, result in variant geopolymer characteristics. Therefore, different trial
mixes with various concentrations of alkaline activators are needed to achieve the target performance for each source. However,
developing a more efficient waste management system focusing on upscaling of CDW rather than the current practice of down
cycling may help in eliminating the effect of this variability.
- The majority of the available investigations used either high dosages of chemical activators, thermal curing treatment or both to
produce CDW-based geopolymers having comparable properties to those with OPC. Such requirements increase the production cost
or make on-site casting impractical.
- High energy required to produce the commonly used activators such as sodium hydroxide and sodium silicate is another obstacle
facing the widespread use of geopolymers. According to Ref. [11], almost 60% of carbon dioxide emissions resulting from geo
polymer concrete are associated with the production of alkaline activators.
- While the utilisation of high concentrations of activators might enhance the mechanical properties of geopolymers, increased
alkalinity can cause some difficulties for the mixtures at fresh state during handling, which necessitates higher contents of
superplasticizers.
- Another aspect to be considered in terms of the development of geopolymer concretes is the possibility of efflorescence formation,
which can be identified as the formation of salt on the surface of concrete. This phenomenon may occur in geopolymers due to the
high content and concentration of alkaline activators. However, the incidence of efflorescence can be minimised by increasing the
content of silica and alumina in the mixtures.
10. Conclusions
The current paper reviewed the fundamental factors that have major influences on the properties of geopolymers produced with
CDW-based materials. Moreover, the main barriers and challenges faced in implementing geopolymers and the steps required to
overcome these issues are also discussed. Following conclusions were drawn:
• Although a few methods for the mix design of geopolymers have been suggested, the trial and error approach is still the most
common one due to large number of parameters involved in geopolymer mix design.
• The use of CDW-based materials rich in silica and alumina, such as bricks and ceramics, resulted in better mechanical performances
than waste concrete; however, superior performance can be achieved by using different sources of CDW-based materials if the
proportions of the activators and heat curing are.
• Higher compressive strengths can be obtained with finer fractions of CDWs, especially if the particle sizes are smaller than 75 μm,
while applying thermal curing in temperature range of 60–90 ◦ C can significantly accelerate geopolymerization, improving the
mechanical performance and durability.
• Geopolymers with only CDW-based fractions as the binder phase exhibited poor mechanical performance under ambient tem
perature curing, whilst the inclusion of SCMs such as GGBFS and MK in CDW-based geopolymers can improve the mechanical
performance with consideration of the influence of other factors such as the decrease in workability. Hence, it seems an essential
factor to use either heat treatment or adding SCM materials for proper synthesis CDW-based geopolymers with acceptable
properties.
• The higher concentration of sodium hydroxide can help improve the mechanical properties of geopolymers; however, the best
possible performances seem to be obtained with molarity range of 8–12 M.
• The use of alkaline activators composed of sodium silicate and sodium hydroxide has been reported as the most effective activators
for enhancing the mechanical properties of CDW-based geopolymer matrices, with a recommended sodium silicate-to-sodium
hydroxide ratio between 1.0 and 2.0.
• The inclusion of higher ratios of sodium silicate decreases the workability of fresh mixtures owing to the high viscosity of Na2SiO3,
whilst increasing the concentration of NaOH can prolong the setting time of geopolymers. The concentration of sodium hydroxide
and the amount of CDW-based materials used also influence the workability and the initial and final setting time of geopolymer
mixtures.
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M. Alhawat et al.
Table 3
Summary of CDWs used as aluminosilicate precursors in the synthesis of geopolymers.
Reference Mix Type Aluminosilicates Activators Curing conditions C.S (MPa) Remarks
[107] paste concrete - NaOH, SS 6, 10, 12, 14, 14 0.5, 1, 20–90 ◦ C for 4, 12, 24, 14.3 The optimal NaOH concentration was 14 M, with SS/NaOH
18 1.5, 2, 48 and 72 h ratio of 1.5.
2.5
[98] binder clay brick, - NaOH 12.4, 14.9, 12 - 50, 65, 75, 85, 95, 105, up to 47 Hollow brick was the most effective CDW, followed by red
hollow brick, 18.6 115, clay brick and roof tile, while glass showed the lowest
roof tile, glass. 125 ◦ C strength.
[175] paste/ CDW-Mix 0, 20% OPC NaOH 6, 10, 11.65 - room temperature for 8.5–18.5 The compressive strength of CDW-based binders activated by
mortar and 24 h Na2SO4 is greater than those activated by NaOH binders at all
Na2SO4 ages.
[176] paste concrete FA-F NaOH, SS 5, 10 10 1, 2 80 ◦ C 7–34.5 The addition of waste concrete up to 50% led to increased
compressive strength for the FA-based geopolymer binders.
[177] paste bricks MK NaOH, SS - 1.4 4 h room temperature, 10–27 Using more waste bricks caused more delay in the yield stress,
then 20 h at 40 ◦ C while using more than 50% of MK led to decreasing the
viscosity of mixes owing to the fast dissolution of MK
particles.
18
[71] paste bricks, concrete - NaOH, SS 12 12 1.0, 1.5 95% RH for 24h, then 10–40 Waste bricks were more reactive during geopolymerzation
soaked in water compared to waste concrete. Increasing the NaOH molarity
led to a significant change in the final setting time of mixtures.
[178] mortar concrete MK, SF NaOH, SS 10 10 1.0 room temperature for 7–27 High polymerization of MK and SF enhanced the low quality
24 h of ITZ in waste concrete-based geopolymers.
[179] paste concrete MK Ca(OH)2, 12 12 1.0 (a) Soaked in water. 1.5–27 Adding calcium hydroxide enhanced the microstructural and
NOH, SS (b) 40 ◦ C/100RH. (c) mechanical properties of CDW-based mixtures. Si/Al ratios
80 ◦ C for 24 h between 3 and 3.8 led to the best properties.
[161] paste ceramic - NaOH, 14 14 2.5 60 ◦ C/95% RH for 24h 26–71 Geopolymers prepared from waste ceramic showed a
SS, KOH reduction in strength after heating at 100 ◦ C for 2 h, while
more increments in temperature until 1000 ◦ C led to
increased strength.
Reference Mix Type Aluminosilicates Activators Curing conditions C.S (MPa) Remarks
[30] paste concrete, brick, SS, KOH 8, 10, 12 12 1.5 room temperature for 3–55 Marine sediments can be partially used with tile and brick for
tile 24h then 60, 80 and producing geopolymers.
90 ◦ C
[31] paste concrete, brick, NaOH, SS 10,12 12 2.0 room temperature for 3–57 Tile and brick showed better mechanical properties
tile 24h then 60, 80 and (50–57 MPa) compared to waste concrete owing to high
90 ◦ C contents of Si and Al. The best performance achieved at 8 and
10 M and at curing temperature of 80–90 ◦ C.
[32] paste clay brick 20–80% NaOH, SS 8 8 2.5 room temperature 3–83 Ambient conditions were insufficient for completing
GGBFS geopolymerization process, reaching 10 MPa as the maximum
strength. The addition of GGBFS to brick-based geopolymer
clearly improved the main characteristics of geopolymers.
[180] paste brick FA NaOH, SS 12 12 1.0 21/50% RH 5–65 The mixture of 50% FA and 50% waste brick showed the best
performance.
[181] mortar ceramic, and - NaOH 6 6 - 24h room 19–48 Ceramic showed better mechanical properties in comparison
clay brick temperature, followed to clay brick due to good bonding of ceramic particles in the
by 40 ◦ C/100% RH matrix.
[182] paste brick, tile, 0–70% NaOH, SS 8, 10, 12 10 - 80 ◦ C for 24h before 2.5–76 The best results obtained by tiles, then bricks, while low
19
concrete, red GGBS curing at room strengths were found in waste concrete based geopolymers. It
mud temperature 7days. is important to balance Si/Ca and Si/Al ratios.
[102] paste concrete 0–30% MK, NaOH, SS 10 10 1.5 (a) room temperature 3–55 The addition of OPC and MK to waste concrete enhanced
OPC (b) 70 C◦ for 24 h, then geopolymerization process.
90% RH
[183] paste brick 0, 20% OPC NaOH, SS 12 12 - (a) room temperature 54–102 The use of 20% OPC led to acquirement of paste with double
(b) 70 ◦ C for 24h strength compared to that produced without OPC, and the use
(c) 70 ◦ C for 48h of hybrid sodium silicate and sodium hydroxide contributed
to the achievement of strengths more than 7 times of that
using sodium hydroxide alone.
[184] mortar bricks, ceramic 5% Ca NaOH, SS 12 12 - 65 ◦ C for 3 days 23–53 The behaviour of the mortar was substantially influenced by
(OH)2 the curing temperature selected.
Reference Mix Type Aluminosilicates Activators Curing conditions C.S (MPa) Remarks
[139] mortar bricks - NaOH, SS 10 10 0.8–2.2 90 ◦ C for 5 days 16- 36 The flowability of mixtures rose with increasing Na2O
concentrations. More pronounced crystal peaks were
observed with increasing bricks in the mixes.
[172] paste bricks OPC NaOH, SS 6, 8 8 - room temperature 10.3–52 The mixture of 70% bricks and 30% OPC exhibited the best
combined performance in terms of environmental impact and
compressive strength.
[24] mortar Bricks, ceramic 0–50% NaOH, SS 12 12 1.0 room temperature 24–93 The high contents of calcium oxide in GGBS significantly
GBGS densified the CDW-based geopolymer matrix.
[28] mortar concrete, 0–50% MK, NaOH, SS 14 14 1.5 room temperature 18 In comparison to OPC-based paste, geopolymers may save
bricks, ceramic, energy up to 45%, and could minimise the greenhouse gas
glass emissions up to 72%.
[25] paste concrete, FA-F, FA-C, NaOH, SS 10 10 - 50, 75, 100 ◦ C 25–58 The flowability rose with increasing the ratios of Na2O/SiO2
bricks, MK, GBGFS and SiO2/Al2O3, whilst setting time shortened with increasing
Na2O/SiO2 and prolonged with higher SiO2/Al2O3.
[99] paste Clay bricks, - NaOH 10, 15, 19 15 - 95, 105, 115, 125 ◦ C 10- 80 Hollow bricks showed the best findings. The main products
20
Table 4
Description of the main factors affecting CDW-based geopolymers [186–191].
• Naphthalene-based superplasticizers are the most advisable high-range water-reducing admixtures for geopolymer systems acti
vated solely by NaOH, whilst polycarboxylate-based plasticizers showed the best plasticizing effect amongst other commercial
superplasticizers available for geopolymer systems activated by both sodium silicate and sodium hydroxide.
In order to address the challenges identified in this review paper, the following strategies and future research needs are proposed:
• There is a lack of studies on the production of CDW-based geopolymer concretes as it can be noted from Table 4, since the previous
works mainly focused on the paste and mortar mixtures.
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M. Alhawat et al. Journal of Building Engineering 50 (2022) 104104
• Further investigations should be made on producing more cost-effective, environmentally friendly activators, preferably manu
factured from waste materials (e.g., waste sodic and waste glass).
• While the inclusion of CDW-based materials in producing geopolymer mixtures can greatly reduce the negative environmental
footprint based on some influencing factors such as transportation and mix design, the nature and amount of the alkaline activator
used are the most dominant factors that need to be considered in terms of cost.
• Issues related to the cost and environmental impact of current activators used in producing geopolymers are still the main chal
lenges that need to be addressed for making real-time and large-scale applications widespread.
• There is an urgent need to standardize methods, specifications, and guidelines for the mix design of geopolymers based on the
divergent characteristics of aluminosilicate precursors and activators used.
• More research is required on synthesising high performance geopolymers with minimal dosages of chemical activators as well as
under ambient curing conditions, without any heat treatment. These steps can significantly contribute to producing sustainable
products with highly reduced costs.
• Further research is needed on the application of advanced analytical models that can help understand the geopolymerization ki
netics, formation of geopolymeric gels based on the source materials used and identifying the key parameters of designing the
mixture to be fabricated.
• More studies on the life cycle assessment of the potential geopolymer mixtures should be conducted to reflect the real economic and
environmental benefits obtained from geopolymers compared to conventional concrete.
• More research is still needed in terms of the durability of geopolymers, particularly in the topics related to shrinkage, freeze-thaw
resistance and chloride-induced corrosion along with the long-term durability properties of CDW-based geopolymers.
• Investigations on the structural performance of CDW-based geopolymers are very limited. In fact, only two research papers are
currently available in the literature, investigating the flexural and shear behaviour of geopolymer concrete beams under ambient
conditions using the four-point-bending test [99,192].
Acknowledgements
This work was supported by the Newton Prize 2020, UK-Turkey award, grant reference number NP2020PB\100026, funded by the
Department for Business, Energy & Industrial Strategy. With thanks to our delivery partners, the British Council, UK and the Scientific
and Technological Research Council, Turkey. For further information, please visit www.newton-gcrf.org/newton-fund/newton-prize/.
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