Journal of Cleaner Production 359 (2022) 132043

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Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Preparation, properties and applications of fly ash-based porous

geopolymers: A review
Xinyu Li a, Chengying Bai a, *, Yingjie Qiao a, Xiaodong Wang a, Kun Yang a, Paolo Colombo b, c
a
Key Laboratory of Superlight Materials and Surface Technology, Ministry of Education, College of Materials Science and Chemical Engineering, Harbin Engineering
University, 150001, Harbin, China
b
Department of Industrial Engineering, University of Padova, Italy, via Marzolo, 9, Padova, Italy
c
Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, 16802, United States

A R T I C L E I N F O A B S T R A C T

Handling Editor: Zhen Leng A very large amount of fly ash is generated from coal combustion, and the high value-added and efficient uti­
lization conversion of this solid waste into a resource remains an issue to be solved. Among the many methods of
Keywords: waste resource utilization, the preparation of porous geopolymers is an effective way to improve the added value
Porous geopolymer of fly ash. In this review, the processes for obtaining fly ash-based porous geopolymers are divided into two
Fly ash
categories: bulk-type (direct foaming, sacrificial template, additive manufacturing, and fast microwave foaming
Porosity
method) and sphere-type (suspension solidification, direct molding, and calcium chloride solution gel method).
Mechanical properties
Thermal properties The synthesis routes, main characteristics (pore structure, porosity), and performance (mechanical and thermal
Adsorption properties as well as adsorption etc.) of fly ash-based porous geopolymers are reviewed, and examples of ap­
plications such as heat insulation, filtration, sound absorption, and pH buffering are presented. Moreover, the
future development prospects of this field are discussed.

1. Introduction
With the continued development of the metallurgical industry,
thermal power generation and other industries, the production of in­
dustrial solid wastes such as slag and dust (e. g. fly ash, bottom ash) are
increasing. Fly ash (FA) occupies a high proportion of all industrial solid
wastes. It consists of fine solid particles in flue gas from coal combustion,
which is also known as soot. Its particles generally range in size from 1 to
100 μm and it is considered a type of hazardous solid waste. By the end
of 2017, the Chinese annual output of fly ash reached 686 million tons,
with a year-on-year growth of 4.7%. Emissions have increased expo­
nentially year by year, ranking first in the world in terms of output, and
China has the largest amount of fly ash emissions in the world. Such a
large amount of fly ash seriously encroaches on the land, pollutes the
soil, water, and the atmosphere, and thereby affects human life(Dhadse
et al., 2008; He et al., 2012; Tiwari et al., 2015). Fig. 1 shows the pro­
duction, comprehensive utilization amounts and utilization rate of fly
ash in China from 2013 to 2019 (Fig. 1(a)) (National Annual Report,
2014, 2015, 2016, 2017, 2018, 2019, 2020), the main chemical
composition (Fig. 1(b)), (Zhang, 2020) and a typical microstructure
(Fig. 1(c)) of fly ash. In recent years, the public environmental problems
caused by fly ash have not only become a hot topic in China but also a
global concern. Under such urgent needs, various industries are trying to
use fly ash as a resource, especially in the fields of construction, agri­
culture, and environmental protection. Many studies have been carried
out, such as their use as a raw material for cement or concrete(Xu and
Shi, 2018), improving soil texture and pH(Basu et al., 2009; Mupambwa
et al., 2015; Ukwattage et al., 2013), synthesizing low-cost adsorbents to
remove pollutants in air and water(Wang and Wu, 2006), extraction of
the precious metals found in fly ash(Ketris and Yudovich, 2009), pre­
paring zeolite molecular sieves(Belviso, 2018; Bukhari et al., 2015), and
porous ceramics(Duan et al., 2012; Yin et al., 2019) as well as other high
value-added applications.
Using solid wastes as the main raw materials for the manufacturing
of porous components is considered a suitable green way to upcycle
them into high value-added products in which a large volume of pores
are capable of fulfilling one or more functional purposes(Bai et al., 2021;
Wang et al., 2021c). Porous materials, including porous ceramics and
glass(Mo et al., 2021; Zhao et al., 2021), porous metals(Jiang et al.,
2021), polymer foams(Qiao et al., 2020), porous carbon materials(Ali
et al., 2019; Xiang et al., 2021), zeolites (Alothman, 2012), porous
metal-organic framework materials (Alqadami et al., 2018), porous

* Corresponding author.
E-mail addresses: chengyingbai@163.com, chengyingbai@hrbeu.edu.cn (C. Bai).

https://doi.org/10.1016/j.jclepro.2022.132043
Received 18 December 2021; Received in revised form 3 April 2022; Accepted 27 April 2022
Available online 3 May 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
X. Li et al.
composites(Azhar et al., 2019), and porous geopolymers(Zhang et al.,
2021) are widely used in many areas, including adsorption, filtration,
catalysis, and thermal insulation in which dense materials are not suit­
able. Previous studies have shown that fly ash can be used as a raw
material to prepare various porous materials, such as porous ceramics
(Fu et al., 2019), porous geopolymers(Chen et al., 2020a), and zeolites
(Han et al., 2020).
Porous geopolymers are materials possessing a high volume of
porosity that has been introduced on purpose. Based on their advanta­
geous characteristics of low energy consumption, low pollution, low
thermal conductivity, good thermal stability, and unique adsorption
characteristics, they have been considered promising novel lightweight
porous materials in recent years(Bai and Colombo, 2018; Zhang et al.,
2021). Since a geopolymer foam does not need high-temperature sin­
tering when curing and its CO2 emissions are only 20% of ordinary
porous cement, it reduces the energy consumption of building materials
during its production, while saving energy and conserving heat in its
applications(Barbosa et al., 2000). It is a green environmentally friendly
material that meets the national “energy saving and emission reduction”
strategic demand. Moreover, porous geopolymers have the character­
istics of adsorbing heavy metal ions and organic dyes and of adjusting
the pH, and they can therefore be widely used in the field of wastewater
treatment(Adewuyi, 2021). And the raw materials for their preparation
can come from a wide range of sources. Not only natural minerals but
also industrial solid wastes containing aluminosilicate including fly ash
(Das and Rout, 2021), bottom ash(Biswal et al., 2020), slag(Rathana­
salam et al., 2020), red mud(Ai et al., 2021), and rice husk ash(Liang
et al., 2022) can be used.
Fig. 2 shows the reaction mechanisms of using alkali-activated fly
ash for the preparation of geopolymers (Fernández-Jiménez et al., 2005;
Singh, 2018). The reactions that occur in the preparation of fly
ash-based geopolymers are very complicated. As shown in Fig. 2(a), the
simplified primary reaction of fly ash-based geopolymer is the conden­
sation between the Si4+ and Al3+ species deriving from the (partial)
dissolution of fly ash by the alkaline activating solution, followed by
complex nucleation, oligomerization, and polymerization, and finally, a
new aluminate-based polymer with an amorphous three-dimensional
network structure is obtained. On one or several particle levels shown
in Fig. 2(b), when the surface of a fly ash particle just begins to come into
contact with the alkaline medium, chemical erosion start at a certain
point on the surface (I) and slowly expands forming larger holes, and the
small particles inside are also exposed, causing the whole particle to
undergo alkaline erosion from the outside to the inside and from the
inside to the outside (II). Consequently, the reaction product is gener­
ated both inside and outside the shell of the sphere, forming a dense
matrix (III). However, this shell forming on the ash particles also pre­
vents their contact with the alkaline medium (Ⅳ). In addition, the above
processes do not occur in a gel, resulting in the possibility of the
Fig. 1. (a) The production, comprehensive utilization amounts and utilization rate of fly ash in China from 2013 to 2019. Data from (National Annual Report, 2014,
2015, 2016, 2017, 2018, 2019, 2020); (b) The main chemical composition (wt%) of fly ash. Data from (Zhang, 2020); (c) A SEM image of as received fly ash (data
from unpublished papers of our research group).
2
Journal of Cleaner Production 359 (2022) 132043
simultaneous presence of several forms in a single slurry: unreacted
particles, particles eroded by alkaline solutions but retaining spherical
shapes, reaction products, etc. (Ⅴ).
According to China National Standard (GB/T 50146–2014), fly ash is
usually divided into F-type fly ash and C-type fly ash. F-type fly ash is
obtained from combustion of anthracite or bituminous coal. C-type fly
ash is generally obtained from lignite and sub-bituminous coal which
contain CaO >10 wt%. Class F fly ash has volcanic ash properties, and
class C fly ash shows some gelation properties in addition to volcanic ash
properties. Chinese fly ash is mainly class C fly ash, and its main
chemical composition and SEM image are presented in Fig. 1(b and c).
The micrograph of fly ash contains a large number of spherical particles,
which interact with alkaline substances during geopolymerization
because the main oxides in their composition are SiO2 and Al2O3(Zhang,
2020). To date, there have been a series of reviews on the preparation
methods of porous geopolymers(Bai and Colombo, 2018; Kovárík and
Hájek, 2019) and geopolymer foam applications(Azimi et al., 2016;
Novais et al., 2020a; Rasaki et al., 2019; Tan et al., 2020), such as heat
insulating materials(Azimi et al., 2016) and heavy metal adsorption
(Rasaki et al., 2019; Tan et al., 2020). However, most of these articles
focus on porous geopolymers with high porosity in general, and there is
no overview of porous geopolymers based on fly ash. Only porous
geopolymers whose proportion of fly ash in the raw materials is greater
than 30 wt% are selected and discussed in this review, in view of the
wide use of fly ash as raw mineral material in geopolymer formation. In
this review, the preparation methods, main characteristics and potential
applications of fly ash-based porous geopolymers are summarized and
discussed, and the current development status of fly ash-based porous
geopolymers is analyzed to provide insights into future developments.
2. Synthesis of fly ash based porous geopolymers
Generally, fly ash-based porous geopolymers are fabricated with
different shapes, such as bulk, membrane, and sphere, to adapt their use
to various practical applications. In this section, both the manufacturing
of bulk/membrane and sphere-shaped components are discussed, and
bulk and membrane ones are grouped together because their prepara­
tion methods are usually similar. Manufacturing methods for geo­
polymer mortar, concrete and composites with porous structure from fly
ash have been well described in previous works (Wang et al., 2021c;
Zhang et al., 2021) and will not be discussed here.
2.1. Synthesis of bulk/membrane-type fly ash-based porous geopolymers
In recent years, researchers have explored several processing ap­
proaches for the synthesis of FA-based porous geopolymers. Generally,
they can be divided into the following ones: (1) direct foaming, (2)
sacrificial template, (3) additive manufacturing, (4) fast microwave
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

Fig. 2. (a) Reaction mechanisms of geopolymers prepared from fly ash (redrawn with permission from Minerals; published by MDPI) (Singh, 2018)(b) descriptive
model of the alkali activation of fly ash according to one or several particle levels (Fernández-Jiménez et al., 2005). (redrawn with permission from Cement and
Concrete Research; published by Elsvier).

foaming or a combinations of the above methods(Bai and Colombo,
2018).
2.1.1. Direct foaming method
The typical direct foaming process of porous geopolymer, widely
used for porous ceramics and lightweight concrete fabrication (Wang
et al., 2021a; Yao et al., 2019) is shown in Fig. 3. The process parameters
and properties of fly ash-based geopolymer foams prepared by the direct
foaming method are summarized in Table 1. The geopolymer foam is
obtained from the wet geopolymer slurry by introducing or generating
gas at room temperature in the form of air, oxygen, hydrogen or carbon
dioxide, and the liquid foam is then set and cured at a slightly higher
temperature. Gas is usually produced by the decomposition of a foaming
agent. These foaming agents can be hydrogen peroxide(Khatib et al.,
2020; Liu et al., 2014a; Szabó et al., 2017; Traven et al., 2021),
aluminum powder(Hajimohammadi et al., 2017; Li et al., 2021) zinc
powder(Kioupis et al., 2021; Li et al., 2021), silica fume(Liu et al., 2020;
Ricciotti et al., 2020), sodium perborate(Chindaprasirt and Rattanasak,
2020; Phavongkham et al., 2020), etc. (Table 1). However, the wet foam
produced by these foaming agents is unstable, so large pores often

Fig. 3. The process flow chart for the direct foaming method. (Optical and SEM image from unpublished data of our research group, with H2O2 as blowing agent
plus surfactant).

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X. Li et al. Journal of Cleaner Production 359 (2022) 132043

Table 1
Process parameters and properties of fly ash-based geopolymer foams prepared by the direct foaming method.
Refs Alumino-silicate Alkali ions Blowing Additive Curing Bulk density (g/ Total Compression Thermal
sources Agents (◦ C) cm3) porosity strength Conductivity
(%) (MPa) (W/(m⋅K))

Feng et al. (2015) CFA Na H2O2 – 55,85 0.24–0.37 74.4–81.2 0.4–1.4 0.07–0.09
Łach et al. (2016) FFA Na H2O2 – 75 0.40–0.64 – 1.9–3.4 0.08–0.13
Xiong et al. (2019) CFA + MK Na H2O2 – 40+ RT 0.56–1.20 41.5–72.5 – –
Novais et al. (2016a) CFA + MK Na H2O2 – 40+ RT 0.44–0.91 60.4–80.9 0.3–5.0 0.08–0.17
Cheng-Yong et al. (2017) CFA Na H2O2 – 29 1.47 – 15.0 –
Novais et al. (2018b) CFA + MK Na H2O2 – 40+ RT 0.39–1.19 40.7–80.6 0.2–8.0 –
De Rossi et al. (2018) CFA + MK Na H2O2 – 20 1.00–1.71 44.4–55.9 2.7–11.9 0.19–0.44
Masi et al. (2014) FA Na H2O2 – 70 0.91–1.40 – 2.9–4.7 –
Ducman and Korat (2016) FFA Na H2O2 – 70 0.61–1.00 37.9–48.1 2.9–9.3 –
Vitola (2020) FFA(+MK) Na H2O2 – 45+RT 0.55–0.75 71.0–76.0 0.8–1.6 –
Liu et al. (2014b) CFA Na H2O2 SDBS 70 0.28–1.59 11.2–63.0 0.7–30.3 –
Masi et al. (2014) FA Na H2O2 Lt 02 70 0.72–0.94 – 1.7–4.6 –
Korat and Ducman (2017) FFA Na H2O2 SDS 70 + 20 0.58–1.34 18.9–54.5 2.6–7.2 –
Hajimohammadi et al. CFA + Slag Na H2O2 SDS + 60 0.66–0.67 – 1.5–1.9 0.25–0.27
(2018) XG
Liu et al. (2016) FFA Na H2O2 OA 80 0.37 – 0.55 –
Kaewmee et al. (2020) FFA K H2O2 OA 80 0.41–0.52 – 0.99–1.69 –
Cui et al. (2018) FFA Na H2O2 CS 60 0.31–0.36 70.0–82.0 1.45–1.6 0.11–0.14
Su et al. (2020a) FFA + cement Na H2O2 CS 80 0.39–0.49 – 0.22–2.22 –
Sanjayan et al. (2015) FFA Na Al – 60 0.40–1.31 – 0.9–0.44 –
(Hlaváček et al., 2015) FFA Na Al – 80 0.42–0.78 – − 6.0 ≤0.15
FFA + RHA K Al – 50 – 39.0–67.0 1.0–16.0 –
Muthu and Ramamurthy FFA Na Al – 70,90 0.75–1.80 – − 9.5 –
(2017)
Kränzlein et al. (2018) FFA Na Al,Zn – RT – – 6.7–40.6 –
Leiva et al. (2019) FFA K Al – 40,70 0.92–1.64 – 3.1–5.2 –
Ducman and Korat (2016) FFA Na Al – 70 0.64–0.74 47.9–58.4 3.3–4.3 –
Masi et al. (2014) FA Na Al 70 0.80–1.42 – 1.7–2.4 –
Rickard and Van Riessen FFA Na Al – 70 0.89–0.93 – 5.5–10.9 0.25–0.39
(2014)
Su et al. (2020b) FFA Na Al – 40 0.60–1.20 – – 0.22–0.70
Kioupis et al. (2021) CFA Na/K Al – RT+80 0.64–1.56 – 2.27–24.18 –
Kioupis et al. (2021) CFA Na/K Zn – RT+80 0.59–1.40 – 1.57–14.90 –
Novais et al. (2018a) FA + MK Na Al OSB 25,40 0.43–0.85 74.0–86.8 0.7–4.3 ≥0.08
Novais et al. (2020b) Na Al OSB 23 0.45–0.68 – 0.9–4 ≥0.09
Masi et al. (2014) FA Na Al Lt 02 70 0.73–0.74 – 2.0 –
Zhao et al. (2010) FFA Na SDBS Glutin RT ≥0.41 – ≥6.8 –
Masi et al. (2014) FA Na Lt 02 – 70 1.18–1.32 – 3.6–7.2 –
Böke et al. (2015) FFA Na NaOCl – 40 + – 34.5–62.1 3.1–3.3 –
60+90
Abdollahnejad et al. (2015) FFA Na NaBO3 – 20 1.15–1.28 – 4.1–6.1 0.11–0.18
Phavongkham et al. (2020) CFA + Slag Na NaBO3 WL RT 0.64–0.82 – 4.3–4.8 0.27–0.32
Korat and Ducman (2020) FFA/CFA Na NaBO3 SDS 70 + 20 0.33–1.18 – 1.0–4.1 0.12–0.36
Alghamdi and Neithalath FFA Na NaHCO3 – 85,100 1.15–1.38 45–55 4.0–15.0 0.29–0.37
(2018)
Kioupis et al. (2018) CFA Na/(Na + Si – RT +80 0.84–1.55 – 2.9–14.9 –
K)
Luna-Galiano et al. (2018) FFA K Si – 40,70 0.97–1.4 – 1.5–12.1 –
Roviello et al. (2020) FFA Na Si – 60 0.33–0.68 – 0.7–5.3 0.15–0.25
Huiskes et al. (2016) FFA + Slag Na AEA – 20 0.88 – 9.7 0.11
Gualtieri et al. (2016) FFA Na SiC – RT – 32.0–52.0 – 0.42–0.486
Huang et al. (2018) CFA Na Foam 45,60 0.23–0.57 77.8–91.1 0.35–2.2 0.05–0.11
Pasupathy et al. (2020) FFA + Slag Na Foam RT 0.57–0.56 67.2–74.8 0.3–0.84 0.25–0.28
Gu et al. (2020) FFA + Slag Na Foam 25 0.35–1.49 1.3–76.7 0.5–44.2 0.02–0.19

Refs = References; CFA = C type fly ash; FFA = F type fly ash; MK = Metakaolin; RHA = Rice husk ash; RT = Room temperature; SDBS = Sodium dodecyl benzene
sulfonate; SDS = Sodium dodecyl sulfate; XG = Xanthan gum; OA = Oleic acidn; CS = Calcium stearate; OSB= Octyl sulfobetaine; Lt 02 = Lightcrete 02; WL = Washing
liquid; AEA = Commercial air entraining agent.

appear in the final porous samples due to coarsening and coalescence
phenomena occurring in the liquid, thereby reducing the microstruc­
tural uniformity and affecting the final performance of the materials. To
solve this problem, other additives, such as surfactants, oil, calcium
stearate, thickeners and particles, are usually introduced into the geo­
polymer slurries (Table 1).
As can be seen in Table 1, hydrogen peroxide is the most commonly
used chemical blowing agent. Feng et al. (2015) prepared fly ash-based
porous geopolymers with type C fly ash and sodium silicate as the raw
materials and H2O2 as the foaming agent, obtaining low density and
high porosity samples (0.24 g/cm3 and 81.2%, respectively), with a
relatively uniform morphology but low compression strength (0.67
MPa). Typically, the pore size of fly ash based foams prepared with only
H2O2 as the foaming agent(De Rossi et al., 2018; Novais et al., 2018b;
Szabó et al., 2017) is not uniform. According to Equations (1) and (2)
(Špalek et al., 1982), it easily decomposes into water and oxygen in an
alkaline environment under unstable thermodynamics. Surfactants such
as sodium dodecyl benzene sulfonate (SDBS)(Liu et al., 2014a, 2014b,
2015), sodium dodecyl sulfate (SDS)(Korat and Ducman, 2017; Xu et al.,
2018), oleic acid(Liu et al., 2016), octylsulfobetaine (OSB)(Novais et al.,
2018a, 2020b), Lightcrete 02(Masi et al., 2014) or a commercial air
entraining agent (Huiskes et al., 2016), have been shown to improve the
microstructure of the foams. Surfactants reduce the surface tension of
wet foams in the geopolymer slurry and stabilize the liquid-gas

4
X. Li et al.
interface, reducing coarsening, drainage and film rupture (Weaire and
Hutzler, 1999) Therefore, when mechanical stirring is applied intro­
ducing air into a slurry (frothing) or when gas is generated in it using
blowing agents, a more stable foam can be formed. Indeed, numerous
studies have shown that surfactants can lead to a better control of cell
size and size distribution, as well as the ratio between open and closed
cells. For instance, Xu et al. (2018) found that the addition of sodium
dodecyl sulfate (SDS/K12) effectively improved the stability of wet
foams, reduced the number of macropores with diameters larger than 2
mm, and caused the pore size distribution to be mostly below 2 mm. The
addition of oleic acid caused the pore walls of the material to have
several irregular openings connecting adjacent cells, thus providing a
highly interconnected pore structure and improved water permeability
(Liu et al., 2016).
H2 O2 + OH − →HO−2 + H2 O (1)
H2 O2 + HO−2 →O2 ↑ + H2 O + OH − (2)
with the aim of achieving a low density geopolymer foams, aluminum is
commonly used(Liu et al., 2017; Ricciotti et al., 2020) or zinc powder
(Kioupis et al., 2021; Li et al., 2021). The reaction of aluminum with
water to produce hydrogen is shown in Equations (3) and (4)(Moham­
madian and Haghi, 2013), but the passivation film covering the surface
of the metal hinders its reaction with water. An alkaline solution, such as
a sodium or potassium hydroxide solution, accelerates the reaction of
aluminum in water to produce hydrogen, as shown in Equation (5)
(Abdullah et al., 2013). Therefore, the alkaline environment of the
geopolymer slurry is a suitable medium for hydrogen generation from
aluminum. Kumar et al.(Muthu and Ramamurthy, 2017) initially found
that when the amount of aluminum powder was less than 0.1 wt%, no
obvious porosity was formed. When the amount of aluminum powder
was increased to more than 0.2 wt%, it was difficult to control the
amount of hydrogen produced, leading to the bursting of many bubbles
with a decrease in porosity. Therefore, the introduction amount of
aluminum powder between 0.1% and 0.2% is more appropriate. In
addition to controlling the amount of aluminum powder, the introduc­
tion of additives can also improve the pore structure and pore size dis­
tribution of the foam, obtaining a more uniform pore size distribution,
higher porosity, and lighter fly ash-based porous geopolymers. The
surfactant octyl sulfobetaine was used by researchers to modify a porous
geopolymer slurry to reduce pore collapse and expand the size range of
interconnecting pores in the cell walls. Novais et al. (2018a) found that
octyl sulfobetaine could increase the volume of porosity of geopolymer
samples foamed with aluminum powder up to 86.8%, obtaining an ul­
tralight porous material with low thermal conductivity. Using micro­
tomography and scanning electron microscopy, Ducman et al.(Ducman
and Korat, 2016) found that the samples foamed with aluminum powder
had higher porosity and larger pores than those foamed with hydrogen
peroxide. In addition to aluminum powder, zinc powder can also be
used, leading to fly ash-based foams(Kränzlein et al., 2018).
2Al + 6H2 O→2Al(OH)3 + 3H2 ↑ (3)
2Al + 3H2 O→Al2 O3 + 3H2 ↑ (4)
2Al + 2OH − + 6H2 O →2Al(OH)−4 + 3H2 ↑ (5)
In addition to hydrogen peroxide and Al or Zn powders, powders
containing metallic impurities, such as silica fume(Shao et al., 2021; Shi
et al., 2020) and silicon carbide(Gualtieri et al., 2016). As shown in
Equation (6), metallic Si present in silica fume reacts with water and
hydroxide in an alkaline environment to produce hydrogen bubbles.
Luna-Galiano et al. (2018) used silica fume waste to replace part of the
fly ash raw material (40% at most) to prepare geopolymer foam. The
study observed that curing solidification at 70 ◦ C compared with 40 ◦ C
could reduce the initial and final setting times and increase the material
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Journal of Cleaner Production 359 (2022) 132043
opening rate and noise reduction coefficient.
Si + 2OH − + H2 O → SiO3 + 2H2 ↑ (6)
Sodium hypochlorite(Böke et al., 2015), sodium perborate(Chin­
daprasirt and Rattanasak, 2020; Korat and Ducman, 2020) and sodium
bicarbonate(Alghamdi and Neithalath, 2018) have also been proven to
be effective in direct foaming because they generate gases upon
decomposition. First, sodium hypochlorite decomposes to produce ox­
ygen, which may react with NaOCl and the carbon in fly ash to produce
carbon dioxide to a certain extent, as shown in Equations (7) and (8)
(Böke et al., 2015). Sodium perborate reacts with water to produce
oxygen, as shown in Equation (9), and the formation of sodium hy­
droxide increases the alkalinity promoting the geopolymerization re­
action (the setting of the geopolymer slurry). Abdollahnejad et al.
(2015) reported that the compressive strength of fly ash-based geo­
polymer foam samples prepared with sodium perborate was approxi­
mately 2 times higher than that prepared with hydrogen peroxide (6
MPa and 3 MPa, respectively), while the thermal conductivity values of
the two samples were relatively similar. Moreover, the use of sodium
perborate powder as a foaming agent leads to lower cost and thermal
conductivity than the use of hydrogen peroxide. Phavongkham et al.
(2020) showed that the introduction of a dishwashing agent as a sur­
factant increased the viscosity of the geopolymer slurry, made the foam
more stable and the pores finer and more uniform, and improved the
compressive strength, thermal properties and flame retardancy of the
material. Sodium bicarbonate, as shown in Equation (10), generates
carbon dioxide, and the hydrolysis reaction of sodium carbonate
(Equation (11)) will form sodium hydroxide, promoting the geo­
polymerization reaction. Experiments show that increasing the curing
temperature from 80 to 100 ◦ C can cause the volume of a foam to in­
crease by about 25%, and its bulk density to drop from 1.4 to 1.1
g/cm3(Alghamdi and Neithalath, 2018).
NaOCl → 2NaCl + O2 ↑ (7)
2NaOCl + C→2NaCl + CO2 ↑ (8)
4NaBO3 + H2 O→2NaOH + Na2 B4 O7 + 2O2 ↑ (9)
Δ
2NaHCO3 →Na2 CO3 + H2 O + 2O2 ↑ (10)
Na2 CO3 + H2 O→NaHCO3 + NaOH (11)
In addition to forming the porous geopolymer by decomposing a
foaming agent inside the slurry, it is possible to directly add a pre-
foamed liquid into the slurry(Agustini et al., 2021; Huang et al., 2018;
Zhang and Wang, 2016; Zhao et al., 2020) or to create pores using gas
pressure, a pressurized foam generator, or other mechanical foaming
methods. For instance, Huang et al. (2018) first generated a liquid foam
using a protein foaming agent and water (mass ratio: 1:100) and then
incorporated it into the slurry by mixing, obtaining an ultrahigh porosity
and ultralight fly ash-based porous geopolymer (total porosity: 91.14%,
volume density: 0.2285 g/cm3).
Foams with improved morphology (more homogeneous pores size)
can also be obtained by employing additives such as xanthan gum (XG)
(Hajimohammadi et al., 2018), calcium stearate (Wu et al., 2018; Xiong
et al., 2019) and starch (C6H10O5)n(Naveed et al., 2019a, 2019b).
Xanthan gum and starch affect the Plateau borders decreasing the
drainage of the liquid because of their thickening ability, and the
increased slurry viscosity leads to a smaller cell size and narrower size
distribution, improving the control of the foaming process(Hajimo­
hammadi et al., 2018). Calcium stearate (CS, see Fig. 8 later) can lower
the surface tension of bubbles and enhance the strength and elasticity of
the bubble shells (Cui et al., 2018).
2.1.2. Sacrificial template method
As shown in Fig. 4, the sacrificial template method is a
X. Li et al.
Fig. 4. The process flow chart of the sacrificial template method.
manufacturing technology that first mixes a proper amount of a sacri­
ficial template filler as the pore-forming material in a geopolymer slurry
to obtain a filler/geopolymer composite material, and then removes the
filler to form a porous geopolymer. The porous material formed by this
method is an inverse copy of the original sacrificial template filler. In the
preparation of fly ash-based porous geopolymers, the sacrificial tem­
plate filler is generally polylactic acid (PLA), which can be removed
from the dual-phase composite by heat treatments, such as thermal
decomposition, melting, dissolution, sublimation or by a chemical
treatment, to produce porosity. The way to remove a template filler from
dual-phase composites mainly depends on the type of filler, and a
combination of two or more removal methods is more effective.
In metakaolin-based porous geopolymers, a more conventional
method is to directly add polylactic acid fibers to the geopolymer slurry
as a sacrificial template filler(Okada et al., 2011; Rasouli et al., 2015),
but Franchin et al.(Franchin and Colombo, 2015) developed a new
processing method combining 3D printing with the sacrificial template
method to manufacture a macro-porous fly ash-based geopolymer with
controllable porosity that was generated based on a CAD design. In this
method, a 3D printer is first used to create PLA (polylactic acid) sacri­
ficial template fillers with different patterns. Next the homogeneous
geopolymer slurry with the PLA fillers is poured into the mold under
vacuum (− 0.1 Pa) and then curing at room temperature for 48–72 h to
obtain a polylactic acid/geopolymer composite material. The last step is
the removal of polylactic acid filler using a combination of chemical
treatment and thermal decomposition to improve the removal effect.
The polylactic acid/geopolymer composite material is immersed in a 15
mol/L KOH solution for 24 h (72 ◦ C) to dissolve and extract part of the
polylactic acid filler. The remaining polylactic acid filler that cannot be
dissolved by alkali treatment is heat-treated (330 ◦ C for 24 h) to com­
plete the removal, thereby generating a metakaolin/FA-based porous
geopolymer with interconnected and regular pores and porosity in the
range of 66–71%.
Fig. 5. The process flow chart of additive manufacturing (direct ink writing).
6
Journal of Cleaner Production 359 (2022) 132043
2.1.3. Additive manufacturing method
Additive manufacturing is a promising technology to produce porous
materials(Guo and Zhou, 2021; Rasaki et al., 2021). Recently, this less
researched method of producing fly ash-based porous geopolymers has
been used to prepare complex structures with controllable pore size and
pore distribution. In the past few years, additive manufacturing (3D
printing) has received considerable attention due to its ability to prepare
components with complex geometries and high precision, maximum
material savings and excellent design flexibility.
Fig. 5 shows a schematic diagram of fly ash based porous geo­
polymers prepared by the additive manufacturing method (direct ink
writing). To use 3D printed fly ash-based geopolymer foams to replace
traditional insulating materials in sandwich wall panels, Alghamdi et al.
proposed a dual porous system (Alghamdi and Neithalath, 2019). The
pores in the foam are smaller, which are realized by a foaming process
based on Lightcrete 02™ surfactant, and the pores between the printed
struts are larger and based on a CAD design. The prepared geopolymer
foam has a porosity of 55–75%, a bulk density of 0.6–1.0 g/cm3, and the
thermal conductivity is close to the effective thermal conductivity of
commercial insulating materials in the range of 0.15–0.25 W m− 1 K− 1.
The material shows sufficient extrudability compressibility, shape
retention and buildability for practical applications thus preparing the
way for the material and the geometric design of 3D printable geo­
polymer cement foams.
2.1.4. Fast microwave foaming method
Fly ash-based porous geopolymers usually need to be cured for a long
time (approximately 24–48 h) in a conventional oven at 20–90 ◦ C.
Therefore, some researchers have developed a microwave foaming
method for synthesizing fly ash-based porous geopolymers with a
shorter curing time. Recently, a large number of reports have found that
microwave energy is an innovative tool that can be used as a heating
source to influence chemical reactions. The advantages of microwave
heating include instantaneous and very fast heating and easy control.
Another advantage is that heat is directly transferred to the material
X. Li et al.
through the interaction with the electromagnetic field at the water
molecule level. Microwaves have the ability to penetrate the interior of
essentially electromagnetic materials in a short time, so the water in the
entire body quickly reaches a higher temperature through volumetric
heating and it evaporates in a short time, thereby generating a foam
structure within the object. It has been reported that microwaves are
used as a powerful tool for the production of polymer foams through
improved heat transfer(Barber, 1983; Sen et al., 2011), and the use of
microwave methods to synthesize fly ash-based geopolymers has been
reported(Chindaprasirt et al., 2013a, 2013b; Graytee et al., 2018;
Jumrat et al., 2011).
Onutai et al. (2016) used household microwave ovens to synthesize
fly ash-based porous geopolymers. The fly ash paste containing SiO2 and
Al2O3 components was mixed with a sodium silicate (Na2SiO3) solution,
and sodium hydroxide at concentrations of 2, 5, 10, and 15 mol/L was
used as the activator for geopolymerization. After mixing the fly ash and
the alkali activator until the mixture was uniform (approximately 1
min), the geopolymer slurry was cured for 1 min at different output
powers of 200, 500, 700, and 850 W using a household microwave oven,
immediately creating a porous geopolymer. The CT and SEM results
showed that at a higher concentration of NaOH, a fly ash-based geo­
polymer with a density of 0.85 g/cm3 and a volume of 5.77 cm3 in
mesopores can be prepared with a power of 850 W. These results
confirm that under higher NaOH concentrations and higher microwave
output power, the temperature of the geopolymer slurry rises immedi­
ately, and aluminosilicate bonds can be effectively formed in the fly
ash-based porous geopolymer within 1 min after solidification.
2.1.5. Embedding lightweight/porous fillers method
An alternative and unconventional way of making pores is the
embedding of lightweight or porous fillers in a matrix aimed at pro­
ducing lightweight materials (Nodehi, 2021).These fillers are exten­
sively available for resin-matrix composites (Qiao et al., 2020) and
metal-matrix composites(Bahl, 2020). The lightweight/porous fillers in
the geopolymeric matrix could be hollow spheres(Bertling et al., 2004;
Hajimohammadi et al., 2019; Yan et al., 2018) or porous particles
(Colangelo et al., 2018). The microstructure of some fly ash also re­
sembles that of hollow spheres(Blissett and Rowson, 2012; Hanif et al.,
2017).
In 2010, a novel fly ash cenosphere was added to a metakaolin-based
geopolymeric slurry, and low thermal conductivity and low density
cenosphere/metakaolin-based geopolymeric composites were obtained
(Wang et al., 2011). Although the content of fly ash as a filler was low,
this work provided a new concept. Another cenosphere was designed to
mix with fly ash and granulated blast furnace slag, and it was found that
the surface of the cenospheres interacted within the reaction of the
geopolymer to generate a strong bond(Hajimohammadi et al., 2019). In
this case, the larger the amount of added hollow spheres, the lighter and
more heat insulating is the resulting foam. The simultaneous introduc­
tion of gas by direct foaming and the incorporation of a certain number
of hollow microspheres has also been investigated. Shao et al. selected
hollow glass spheres, H2O2 and calcium stearate to achieve very low
density, relatively high strength, and ultralow thermal conductivity,
which was the result of the incorporation of hollow glass spheres to
further control the characteristics of the pore walls(Shao et al., 2018).
2.2. Synthesis of fly ash-based porous geopolymer spheres
Based on the unique characteristics of porous fly ash geopolymers,
research on treating wastewater with such an adsorbent has attracted
extensive attention. Compared with powders and bulk-type adsorbents,
spheres can have several advantages (please refer to Section 3.7 for
further details). Consequently, in addition to the above methods of
preparing bulk-type fly ash-based porous geopolymers, there are several
ways to prepare porous fly ash-based geopolymer spheres, such as the
suspension solidification method, the direct molding method, and the
7
Journal of Cleaner Production 359 (2022) 132043
calcium chloride solution gel method.
2.2.1. Suspension solidification method
The suspension solidification method is derived from the suspension
polymerization method. This method is generally used to synthesize
polymer organic microspheres or microbeads (with a particle size range
of 10 μm–5000 μm), and it is suitable for materials that are liquids with a
low density, and that are capable of rapid reaction curing. At present, it
has mature applications in the synthesis of polystyrene and styrene
microspheres. As shown in Fig. 6, the suspension solidification method
uses a water-based geopolymer slurry as the dispersed phase to be sus­
pended in an oil continuous phase. Because the oil and water phases are
incompatible and their densities are close, the dispersed phase droplets
maintain a perfectly spherical shape in the continuous phase under the
action of interfacial tension, and the obtained spheroids have high de­
gree of symmetry and sphericity.
In general, the density of the geopolymer slurry is larger than that of
the continuous phase, approximately 1–2 g/cm3. It is necessary to
combine the density and viscosity to find an oil-based continuous phase
that can stably suspend the slurry droplets. Thus far, polyethylene glycol
600 (Novais et al., 2017, 2018c, 2019; Shimizu et al., 2020) has mainly
been used as the continuous oil phase to prepare fly ash-based porous
geopolymer spheres. In addition, to increase the suspending ability of
the geopolymer slurry droplets, their density can be adjusted by adding
foaming agents, such as sodium lauryl sulfate (Novais et al., 2017,
2018c, 2019), Tween 80 and hydrogen peroxide (Shimizu et al., 2020).
By adding a foaming agent, not only can the density of the slurry be
adjusted but also the porosity of the geopolymer after solidification can
be modified, to obtain geopolymer materials with different geometric
surface area and pore structure. The temperature of the water bath is
generally between 85 and 90 ◦ C, so that the slurry can quickly solidify
into spheres in the oil continuous phase, with a particle size in the range
of 2–4 mm.
2.2.2. Direct molding method
According to the current literature, most geopolymer spheres are
produced through additional suspension and solidification steps, but the
easier-to-operate direct molding method should also be considered to
prepare spheres. Tan et al. (2021) selected fly ash and calcined kaolin
(mixed in a ratio of 2:1 by weight) as the source of aluminosilicate,
added an alkaline activator and water, followed by the addition of H2O2
(1.2 wt%). Immediately after mixing, the fresh sample was poured into a
spherical mold and cured at 60 ◦ C for 24 h. To prevent excessive
evaporation of water, the mold was sealed with a polyethylene film. The
direct molding method is not only simpler and easier to operate than the
suspension solidification method, but it also does not have the strict
requirements on the density and viscosity of the slurry and can prepare
porous geopolymer spheres with a wider density range.
2.2.3. Calcium chloride solution gel method
The calcium chloride solution gel method utilizes Ca2+ to form a
three-dimensional network structure with the G unit in the alginate
when the foamed geopolymer slurry is in contact with alginate in the
solution(Isabelle Braccini, 2001). Nurddin et al. manually stirred and
mixed NaOH solutions of different concentrations with fly ash, poured a
sodium alginate solution (2.0 wt%) into the geopolymer slurry, and
mixed at 500 rpm for approximately 30 min. Then, a protein was added
to the slurry and mixed evenly to foam it, and the slurry was then added
dropwise to the CaCl2 solution (2 wt%). The formed microspheres were
kept in the solution at room temperature for 24 h. Through methylene
blue (MB) adsorption experiments and response surface methods, it was
found that the protein content was the most effective factor improving
the adsorption performance, followed by curing temperature and so­
dium alginate dosage(Nurddin et al., 2020).
According to the above analysis, the features, advantages, and dis­
advantages of different method are compared and listed in Table 2. For
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

Fig. 6. The process flow chart of the suspension solidification method. (Optical image from unpublished work of our research group).

Table 2
The features, advantages and disadvantages of different fabrication methods.
Shape Method Features Advantages Disadvantages Ref

Bulk- DFM Gas from blowing agent or mechanical Relatively homogeneous pore Thermodynamically unstable process (Kaewmee et al., 2020; Khatib
type frothing structure Extremely wide pore size distribution et al., 2020; Traven et al., 2021)
Simple preparation procedure
Easy large-scale production
High porosity
STM Negative replica of the original template Controllable pore geometry Required extra step for templates Franchin and Colombo (2015)
removal and sometimes harmful
Limited fabrication for large parts
Long processing times
ADM Designability with 3D printer Precisely control the pore Rheology requirements of slurry for Alghamdi and Neithalath (2019)
shape, dimension, and amount shape retention and buildability
Connected macroporous Short printing window time
structure
FMFM Microwave foaming Fast and facile process Inhomogeneity in pore structure Onutai et al. (2016)
ELFM Lightweight/porous fillers addition Closed pore structure Commonly has lower porosity (Hajimohammadi et al., 2019;
High mechanical strength Nodehi, 2021)
Sphere- SSM Interfacial tension High specific surface area Density requirements of slurry (Novais et al., 2017, 2018c, 2019)
type Small size samples Contain organic matter
Limited and lower porosity
DMM Spherical shape by mold Relatively simple preparation Sphericity controlled by mold Tan et al. (2021)
procedure
2+
CCSGM Ca to form a three-dimensional High specific surface area Lower high-temperature stability Nurddin et al. (2020)
network structure with the G unit in the Small size samples High cost
alginate Contain organic matter

DFM = Direct foaming method; STM=Sacrificial template method; ADM = Additive manufacturing method; FMFM=Fast microwave foaming method; ELFM =
Embedding lightweight/porous fillers method; SSM=Suspension solidification method; DMM = Direct molding method; CCSGM=Calcium chloride solution gel
method.

the bulk/membrane-type fly ash-based porous geopolymers, the direct the macro-pore size and distribution can be regulated with the addition
foaming route was the most common method as well. (Kaewmee et al., of stabilizing agents. Besides, a high porosity up to 91 vol% can be
2020; Khatib et al., 2020; Traven et al., 2021). Although foaming using achieved (Table 1), (Huang et al., 2018) and the facile preparation
artificially made gas bubbles is a thermodynamically unstable process, procedure is expected to easily enable large scale continuous

8
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

production. With respect to the sacrificial template method, the pore
shape and size are determined by the template, and there are only a few
of templates (e.g., polylactic acid, NaCl) (Franchin and Colombo, 2015;
Wang et al., 2021) that are practicable for porous geopolymer forma­
tion. Moreover, the templates require complex steps and/or long time or
high temperature treatment to extract, especially for larger parts. 3D
printing was explored to produce porous geopolymers with designed
shapes, allowing a better control of the pore shape, dimension, and
amount. Despite the interesting possibilities offered by 3D printing, the
demanding slurries’ rheology and short printing window time can be
quite a challenge in future applications (Alghamdi and Neithalath,
2019). Although the pores of samples prepared by microwave foaming
method was not as uniform as other methods, it deserves more attention
due to the rapidity, convenience, and lack of any foaming agents(Onutai
et al., 2016). The embedding lightweight/porous fillers method was also
reported to obtain a high mechanical strength with lightweight/porous
fillers addition(Hajimohammadi et al., 2019; Nodehi, 2021).
On the other hand, there are three methods for fabricating sphere-
type fly ash-based porous geopolymers. The suspension solidification
method has been widely used to prepare spherical geopolymer foams
due to its high specific surface area and small particle size. However,
engineering challenges associated with the density requirements of
slurry, content of organic matter and limited porosity cannot be
neglected (Novais et al., 2017, 2018c, 2019). The direct molding method
is based on the direct foaming route and differs from the suspension
solidification method because of the use of a mold to provide the
spherical shape; the direct molding method makes greater demands of
the stability of the foamed slurry than other routes (Tan et al., 2021).
Finally, although the calcium chloride solution gel method has been
rarely investigated, samples prepared via this method had high specific
surface area despite the high cost and painstaking process (Nurddin
et al., 2020). It should be noted that the features discussed in Table 2 are
not restricted to fly ash-based porous geopolymers, as there are not
sufficient examples of the use of fly ash for each foaming method.
3. Properties and potential applications of fly ash-based porous
geopolymers
In this section, the pore structure, density, porosity, compressive
strength, thermal insulating properties, high temperature properties,
flame retardant properties, sound absorption properties, adsorption
properties, and pH regulating ability of fly ash-based porous geo­
polymers are reported. Factors affecting the properties of fly ash-based
porous geopolymers are the focus, therefore geopolymer mortar/con­
crete composites filled with sand or other aggregates and phase transi­
tion composites will not be discussed in this review.

Fig. 7. Fly ash-based porous geopolymers with uniform pore distributions prepared by using different foaming agents and additives. (a) Al(Hlaváček et al., 2015)
(Reproduced with permission from Journal of the European Ceramic Society; published by Elsevier); (b) Al + OSB(Novais et al., 2018a) (Reproduced with permission
from Ceramics International; published by Elsevier); (c) NaBO3(Phavongkham et al., 2020) (Reproduced with permission from Construction and Building Materials;
published by Elsevier); (d) Foam(Huang et al., 2018) (Reproduced with permission from Energy & Buildings; published by Elsevier); (e) Si(Škvára et al., 2014)
(Reproduced with permission from Ceramics–Silikáty; published by University of Chemistry and Technology, Prague; Institute of Rock Structure and Mechanics of
the CAS); (f) SDBS (Zhao et al., 2010) (Reproduced with permission from Journal of Hazardous Materials; published by Elsevier); (g) H2O2(Feng et al., 2015)
(Reproduced with permission from Materials and Design; published by Elsevier); (h) H2O2+SDS(Korat and Ducman, 2017) (Reproduced with permission from
Cement and Concrete Composites; published by Elsevier).

9
X. Li et al.
3.1. Pore structure
The pore size range of fly ash-based porous geopolymers is mostly in
the millimeter-scale, and the foaming methods discussed above will
affect the pore characteristics of porous geopolymers, including their
size, volume, shape and connectivity. As shown in Fig. 7, in the direct
foaming method the pore characteristics obtained by different foaming
agents are also different. Compared with the use of Al powder, adding
H2O2 tends to produce more spherical cells and a narrower cell size
distribution, leading to a more homogeneous microstructure, but
because of all the different preparation technologies employed in the
literature, the research on pore size formation still has no unified con­
clusions(Ducman and Korat, 2016; Masi et al., 2014). The use of the
foaming agent affects the pore size to a great extent, as does the material
itself. For example, with an increase in the content of H2O2, the size of
the cells is reduced, and the number of pores is relatively large (Feng
et al., 2015; Korat and Ducman, 2017; Liu et al., 2014a; Novais et al.,
2016a, 2016b; Xu et al., 2018).The size of the cells in important for two
reasons: on the one hand, an increase of the H2O2 leads to an increased
chance of coalescence between adjacent cells, with smaller pores being
absorbed into larger ones increasing the risk of forming macropores. On
the other hand, with the increase in the amount of H2O2 added, the
amount of water generated by decomposition increases, the viscosity of
the slurry decreases and the fluidity increases. Sometimes, during the
foaming process the ultimate shear stress of the wet foam increases too
quickly, resulting in bubbles merging into large ones over a small range
(Xu et al., 2018). With increasing cell diameter, the resulting foam has
more openings and stronger connectivity, but reduced strength. The
presence of interconnecting pores gives the sample a high geometric
surface area that increases its water absorption, which is not good for
thermal insulation but improves the material’s potential for adsorption
applications. In addition, the amount of sodium silicate(Feng et al.,
2015) and the molar concentration of sodium hydroxide(Novais et al.,
2016a) can also affect the pore structure of fly ash-based porous
geopolymers.
To obtain a more uniform pore size distribution of fly ash-based
porous geopolymers, it is necessary to add surfactants and other
external additives, such as foam stabilizers. Cui (Cui et al., 2018)
confirmed, as shown in Fig. 8, that at the same environmental temper­
ature, calcium stearate (CS) can significantly reduce the surface tension
of the geopolymer slurry bubbles. When the calcium stearate increased
from 0.5% to 1.0%, the surface tension was significantly reduced from
86 mN/m to 54 mN/m and then decreased to 33 mN/m. The higher
surface tension of the base activator without calcium stearate is not
conducive to the formation and stability of bubbles, because a gas-liquid
film with a higher surface tension is prone to rupture or coalescence,
thus reducing the surface free energy. When sufficient calcium stearate
is present, the surface tension of the gas bubbles decreases, and the
strength and elasticity of the bubble shell increases to avoid the
Fig. 8. (a) The variation of surface tension without and with calcium stearate (CSFS); (b) Schematic diagram of the bubble strengthening/pore stabilizing process
(Cui et al., 2018).(Reproduced with permission from Journal of Building Engineering; published by Elsevier).
10
Journal of Cleaner Production 359 (2022) 132043
formation of large voids. Numerous studies have shown that these ad­
ditives can better control the cell size and the size distribution as well as
the ratio of the open and closed cells (Cui et al., 2018; Hajimohammadi
et al., 2018; Kaewmee et al., 2020; Korat and Ducman, 2017; Traven
et al., 2021).
The pore characteristics of fly ash-based porous geopolymers pre­
pared by the sacrificial template method are mostly dependent on the
shape of the template, and the template removal method may also have a
certain effect. The design capability of the additive manufacturing
method greatly increases the range of pore structures achievable,
moreover providing a very uniform distribution of pore sizes. In addi­
tion, an increase in the molar concentration of sodium hydroxide and
microwave power can increase the number of open pores of fly ash-
based porous geopolymers prepared by microwave foaming(Onutai
et al., 2016).
3.2. Porosity and compressive strength
Table 1 reports that the density of fly ash-based geopolymers pro­
duced using the direct foaming method ranges from ~0.24 to <2 g/cm3.
Most of the samples have total porosity values between 40 and 80 vol%,
and the density and porosity show an obviously inverse relationship so
that when the porosity increases the density decreases.
For porous fly ash-based geopolymers prepared by the direct foaming
method, their density and porosity depend mainly on the content of
foaming agent and the slurry viscosity, and therefore also on the pa­
rameters that directly affect the rheology and reactivity of the mixture,
such as the content of foaming agent(Ducman and Korat, 2016; Feng
et al., 2015; Gu et al., 2020; Huang et al., 2018; Korat and Ducman,
2017; Novais et al., 2016a, 2018a, 2018b; Pasupathy et al., 2020), the
type of foaming agent(Ducman and Korat, 2016; Kioupis et al., 2021;
Masi et al., 2014), the alkali activator content(Huang et al., 2018;
Novais et al., 2016a), the liquid content (liquid-solid ratio)(Novais et al.,
2018a), the fly ash particle size(Xiong et al., 2019), the curing temper­
ature(Huang et al., 2018), etc. It is well known that the porosity will
increase with increasing the content of foaming agent, but research
shows that there is a critical value for its amount; that is, when the
critical value is exceeded, porosity will decrease. The critical value is
mainly related to the viscosity of the slurry because a high viscosity
slurry is not conducive to pore expansion(Ducman and Korat, 2016;
Feng et al., 2015; Gu et al., 2020; Huang et al., 2018; Korat and Ducman,
2017; Novais et al., 2016a, 2018a, 2018b; Pasupathy et al., 2020).
The mechanical strength of porous materials depends largely on their
porosity, and the relationship between strength and porosity has been
studied based on several established models(Lian et al., 2011; Rice,
1993, 1996; Ryshkewitch 1953). The model first proposed byRyshke­
with (1953) and further improved by Rice(Rice, 1993, 1996) has been
widely used to study the strength-to-porosity relationship. This model,
also known as the minimum solid area (MSA) model, is based on the
X. Li et al.
assumption that the mechanical behavior of the specific porous solid
ideally corresponds to that of a cellular material with a structure
comprising the dense uniform packing of identical spherical (or cylin­
drical) cells. The fitting of experimental data is obtained by referring to a
particular way of packing or stacking of individual cells and taking into
account their shape, as follows:
σ = σ0 e − bp
(12)
where σ is the strength of the material, σ 0 is the strength of the same
material without porosity, and b is a constant depending on the partic­
ular packing/stacking of spherical or cylindrical pores. Fig. 9 shows the
variation of the compressive strength as a function of the total porosity
of the fly ash foams obtained from different processing routes and with
different compositions. The model has been validated for metakaolin-
based porous geopolymers (Bai et al., 2016, 2017; Bai and Colombo,
2017; Franchin et al., 2017; Palmero et al., 2015), but no obvious trend
can be discerned from Fig. 9. The reason is that the parameters such as
raw material composition, degree of oligomerization, NaOH/Na2SiO3
ratio, NaOH concentration, water content, curing temperature and so on
are not the same for each study, which makes the data not directly
comparable in a straightforward manner as the intrinsic strength of the
geopolymer matrix changes. However, the influence of different pa­
rameters on the material strength can be summarized.
The parameters that affect the density and porosity of fly ash-based
porous geopolymers can affect the strength of the material and, for a
foam, the amount of added foaming agent is the most influential factor.
Increasing the content of almost all types of foaming agents results in a
reduction of strength and a decrease in density, which is the expected
result due to the higher amount of porosity present in the samples(Feng
et al., 2015; Gu et al., 2020; Huang et al., 2018; Novais et al., 2016a,
2018a).
Several synthesis parameters can effectively improve the strength of
a geopolymer, i.e. the amount of geopolymer gel is known to affect the
compressive strength of the material(Duxson et al., 2005). In the syn­
thesis of FA-based geopolymers, when the solid/liquid ratio (S/L) of the
initial mixture was increased, the compressive strength of the material
increased almost exponentially until S/L = 2.05 kg/L and then it
decreased sharply(Panias et al., 2007); that is, when the liquid content is
low, the compressive strength of the material is high, and the higher the
fly ash content is, the higher the compressive strength is. An increase of
the sodium silicate/potassium sodium silicate ratio can increase the Si
content, water content and SiO2/Al2O3 ratio, while an increase in the
Fig. 9. Relationship between compressive strength and total porosity of fly ash-
based porous geopolymers.
11
Journal of Cleaner Production 359 (2022) 132043
SiO2/Al2O3 ratio leads to an increase in Si–O–Si bonds, and the Si–O–Si
bonds are stronger than the Si–O–Al bonds. CaO from the FA or added to
the initial mixture can also affect the final compressive strength of a
geopolymer foam. It has been reported that the addition of CaO and Ca
(OH)2 can improve the compressive strength of the prepared fly ash
based polymer, which may be attributable to the precipitation of cal­
cium silicate hydrate or calcium silicate aluminate hydrate phases
(Abdollahnejad et al., 2015; Temuujin et al., 2009).
3.3. Thermal insulating properties
In general, the coefficient of thermal conductivity of a geopolymer
foam is mainly associated with the porosity and pore distribution of the
material(Batool et al., 2018; Sengul et al., 2011). The increase in
porosity decreases the volume of the solid skeleton structure, and since
its thermal conductivity is much higher than that of air it enables the
geopolymer foams to provide a higher heat insulation (Cui et al., 2018;
Hassan et al., 2018). In other words, the thermal conductivity decreases
with increasing porosity (see Fig. 10(a)), as is generally the case with
other porous materials(Feng et al., 2015). Therefore, the factors
affecting the porosity mentioned in Section 2.1 will affect the thermal
conductivity of the geopolymer foams to a certain extent; the discussion
will not be repeated here.
A fly ash-based porous geopolymer can be regarded as a two-phase
system composed of a solid skeleton and voids. The effective thermal
conductivity of the two-phase composite material (the fly ash-based
polymer matrix and the voids) can be predicted by using several ther­
mal conductivity models. For example, simple parallel and series
models, the Maxwell-Euchen 1 (ME1) model, the Max Well-Euchen 2
(ME2) model, and the effective medium theory (EMT) model are shown
in Fig. 11, but how to choose an appropriate model depends on several
microstructural factors(Awad and Muzychka, 2008; Feneuil et al., 2017;
Smith et al., 2013; Troschke and Burkhardt, 1998). The horizontal line
in Fig. 10(b) corresponds to the thermal conductivity of commercially
available insulating materials, as a reference. When the air volume
fraction is approximately 60–70 vol%, the effective medium theory
(EMT) predicts that the geopolymer foam will have thermal conductivity
values similar to those of commercial insulating materials(Alghamdi and
Neithalath, 2019); however, the data reported in Fig. 10 indicate that
this is not the case in real samples, as a much larger volume of porosity is
required to achieve such low conductivity values.
The pore size distribution and pore network connectivity also in­
fluence the thermal conductivity, and a narrower pore distribution en­
ables the material to have good insulation performance. Some additives,
such as surfactants, have a large effect on the pore size distribution and
will affect the foam’s thermal properties(Hajimohammadi et al., 2018).
Cui et al. (2018) explored the influence of calcium stearate on thermal
conductivity and found that when the calcium stearate content was 1%,
the thermal conductivity dropped to the lowest value (0.095 W m− 1
K− 1), and the total porosity reached the highest value (82%). When the
content calcium stearate is different from 1%, the decrease in the ther­
mal conductivity can be explained by an increase in micropores, and the
effect is called the Knudsen effect(Jelle et al., 2010). For the Knudsen
effect to work, the pore has to be very small, preferably in the nanometre
range. The smaller the aperture is, the larger the Knudsen effect. The
Knudsen effect begins to become effective when pores have a size be­
tween 10 μm and 1 μm (0.021–0.025 W m− 1 K− 1), and is more pro­
nounced for pores with a size between 1 μm and 100 nm (0.008–0.021
W m− 1 K− 1), with the most benefit arising when the size is below 100 nm
(0.002–0.008 W m− 1 K− 1) (Jelle et al., 2010). This means that under the
same total porosity, the higher the microporosity is, the smaller the
thermal conductivity is. The pore connectivity also affects the thermal
conductivity of fly ash-based geopolymer foams to a certain extent.
When the amount of the connected pores increases, the thermal con­
ductivity of the material will also increase(Gu et al., 2020).
Fly ash-based porous geopolymers exhibit lower thermal
X. Li et al.
Fig. 10. (a) Relationship between the thermal conductivity and total porosity of fly ash-based porous geopolymers; (b) Several analytical several analytical models
for the measured and effective thermal conductivity of geopolymer foams(Alghamdi and Neithalath, 2019). (Reproduced with permission from Cement and Concrete
Composites; published by Elsevier).
Fig. 11. Relative mass, relative volume, and color of porous FA-based geo­
polymers as a function of heating temperature(Hlaváček et al., 2015). (Repro­
duced with permission from Journal of the European Ceramic Society;
published by Elsevier).
conductivity than some insulation materials, which proves the feasi­
bility of their application in the field. However, two things still need to
be considered. First, fly ash-based geopolymer foams have a high water
absorption rate, and water (in the form of adsorbed humidity) will
greatly increase the thermal conductivity of the materials. Second, high
porosity and low coefficients of thermal conductivity of porous fly ash-
based geopolymer are always accompanied by a partial loss of their
material strength. The recently studied double-layer porous cork/fly
ash-based polymer composites can to a certain extent address the
problems stated above (Novais et al., 2020b).
3.4. High temperature and flame retarding properties
Studies show that when fly ash-based polymer foams are heated up to
1000 ◦ C, no significant thermal degradation phenomena occur. Above
1000 ◦ C, cracks form due to crystallization and shrinkage, and pore
interconnectivity increases, affecting the strength of the samples. After
the heat treatment, the color of the geopolymer will change (<1000 ◦ C),
and the inner surfaces of the pores will change from smooth to rough,
because of the formation of crystals. Fig. 11 shows the changes in vol­
ume, mass and color of sample after the high-temperature test. It can be
observed that the mass loss during sintering is small, and the loss is due
12
Journal of Cleaner Production 359 (2022) 132043
mainly to various forms of water(Hlaváček et al., 2015). In geopolymers,
water may exist in the form of free adsorbed water in micropores and gel
pores and also in the form of OH groups at the end of the Si–O–Si chains.
The water in the gel pores is bound in the form of Na(H2O)+. More than
60% of the H2O (mainly free water) is lost when heating to temperatures
below 200 ◦ C. When the material is heated to a temperature higher than
200–300 ◦ C, the chemically bound OH groups condense forming T-O-T
bonds and, at the same time, the alkaline cations are shifted, leading to a
change in the microstructure. Almost all chemically and physically
bound water is lost by 800 ◦ C. The volume shrinkage increment, which is
the largest between 800 and 1100 ◦ C, is related to gel sintering, with the
loss of the mesopores.
The material composition also changes during the high-temperature
treatment. In general, geopolymers are either semi-crystalline or
amorphous, and the aluminosilicates used in synthesis contain small
amounts of highly crystalline impurities such as muscovite, quartz, and
corundum. Liu et al. (2015) found that at 70 ◦ C, a fly ash based geo­
polymer foam activated with a Na alkaline solution and with a
SiO2/Al2O3 mole ratio of 3.8 contained quartz, mullite and zeolite as
reaction products. The main phase of the geopolymer system was still an
amorphous material, and the broad peak in the 20–40◦ (2θ) range is
characteristic of amorphous gels, which are mainly N-A-S-H gels. After
sintering at 800–1000 ◦ C, crystal phases of quartz, carnaite, nepheline,
and zeolite were evident in the geopolymer matrix, which may have
contributed to the good strength values. The experiment also proves that
after sintering, the strength of the fly ash-based geopolymer foams is
generally higher than that of the as prepared ones, and the increase in
strength may also be due to the sintering of the aluminosilicate geo­
polymer matrix with unreacted fly ash, which leads to the enhancement
of the connectivity of the particles(Rickard et al., 2011).
Based on the fact that the fly ash-based geopolymer foams increase in
strength after exposure to high temperature, it is suggested that the
material may develop a better structure when exposed to fire. This
unique property will make it possible for geopolymer foams to be used as
refractory material. Recent fire test results, reported in Fig. 12, show
that when the hot side temperature rose to 1000 ◦ C and above, the
temperature of the cold side slowly rose from 35 to 70 ◦ C in 20 min, and
then flattened out over 90–100 min rising to 90 ◦ C, and by 120 min it
quickly reached 240 ◦ C. After 180 min, the temperature of GFS gradually
increased to approximately 300 ◦ C. The slow rise in temperature after
long-term exposure to high temperature indicates that the fly ash-based
geopolymer foam possesses flame retarding characteristics(Phavongk­
ham et al., 2020).
3.5. Sound absorption
To date, there have been only a few studies on the acoustic properties
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

Fig. 12. (a)Optical characters after the fire resistance test and cooling down, temperature on (b) the hot side and (c) the cold side of FA-based geopolymer foams
produced with varying amounts of surfactant (Phavongkham et al., 2020).(Reproduced with permission from Construction and Building Materials; published
by Elsevier)

of fly ash-based geopolymer foams(Leiva et al., 2019; Luna-Galiano
et al., 2018; Shi et al., 2020; Stolz et al., 2018; Zhang et al., 2015), but
they do provide valuable information for their use as sound insulation
materials. The volume density and porosity(Leiva et al., 2019), curing
temperature(Luna-Galiano et al., 2018), raw material type(Zhang et al.,
2015), activating solution(Luna-Galiano et al., 2018) and sample
thickness(Zhang et al., 2015) as well as other parameters were investi­
gated, and their influence on the sound absorption discussed. Zhang
et al. (2015) found that some of the materials prepared by them showed
strong absorption (sound absorption coefficient = 0.7–1) at low

Fig. 13. (a) Images of the samples; (b–d) sound absorption coefficient of fly ash-based porous geopolymers prepared with different process parameters(Luna-Galiano
et al., 2018). (Reproduced with permission from Journal of Non-Crystalline Solids; published by Elsevier)

13
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

frequency (40–150 Hz), a certain amount of sound absorption at
1200–1600 Hz, and poor absorption at 150–1200 Hz. The addition of
30% slag had no obvious effect on the sound absorption in the
low-frequency area and only improved the sound absorption coefficient
of 800–1200 Hz. As shown in Fig. 13, Luna-Galiano et al. (2018) also
observed similar sound absorption characteristics with high absorption
at low frequencies of 125 Hz and 250 Hz and very low absorption in the
range of 500 Hz–2000 Hz. As the frequency was further increased to
4000 Hz and 6300 Hz, the absorption coefficient increased again.
Different studies have shown that the fly ash addition to a porous geo­
polymer improves absorption properties in the low frequency range.
High absorption of low frequency sound is also beneficial for the health
of the human body, as sound in the frequency range of 10–200 Hz is
harmful to people(Leventhall, 2004).
Increasing the thickness of the sample can increase the sound ab­
sorption in this range, but the sound absorption effect is not obvious in
the high frequency range(Zhang et al., 2015). As mentioned earlier,
acoustic properties are closely related to the porous structure of fly
ash-based porous geopolymers, as sound absorption is closely related to
the frictional energy loss at the pore walls of the porous material,
through which sound waves can propagate and decay within the ma­
terial (Arenas et al., 2015, 2017a, 2017b). In terms of porosity, only
open porosity is conducive to acoustic absorption, but if the open
porosity is very high, the effect of the porous structure on sound trans­
mittance will be reduced, thus decreasing the sound absorption perfor­
mance(Maderuelo-Sanz et al., 2016).
3.6. Adsorption
Geopolymers are also considered promising adsorptive materials due
to the ability of the free alkali metal ions in the skeleton to exchange
cations within a solution. As shown in Table 3 and Fig. 14, there have
also been many studies on the adsorption capacity of fly ash-based
porous geopolymers. It has been proven that they can adsorb metal
cations such as Cu2+(Duan et al., 2016; Onutai et al., 2019), Pb2+(Han
et al., 2020; Novais et al., 2016d; Onutai et al., 2019), Cd2+(Onutai
et al., 2019), Ni2+(Onutai et al., 2019) and the organic dye methylene
blue(Liu et al., 2016; Novais et al., 2018b, 2019; Shao et al., 2020).
In addition to heavy metal ions, in 2016 Liu et al. (2016) prepared a
geopolymer foam with variable permeability and a highly inter­
connected pore structure using fly ash, which had a high adsorption
capacity for methylene blue (50.7 mg/g). This study demonstrated the
great potential of fly ash-based porous geopolymers as adsorbents of
methylene blue instead of activated carbon.
To date, scholars have studied the influence of parameters such as
the initial concentration of methylene blue(Novais et al., 2018b, 2019),
adsorbent dosage(Novais et al., 2019) and porosity(Novais et al., 2018b)
on the adsorption of methylene blue by fly ash-based porous geo­
polymers. With the increase in the initial concentration of methylene
blue, the absorption of methylene blue by the porous geopolymer
increased significantly, which was reflected in the gradual increase in its
adsorption capacity. However, since the initial concentration will affect
many factors, such as the number of active sites, the mass transfer
resistance between adsorbents and adsorbents (solid and liquid), and all
these factors will cause a change in removal efficiency, the change in
removal efficiency with the initial concentration is uncertain(Novais
et al., 2018b, 2019). When the amount of adsorbent increased, the ab­
sorption of methylene blue decreased, and the removal efficiency
increased(Novais et al., 2019). The porosity of the geopolymer also
affected the removal of methylene blue, and the higher porosity led to
more methylene blue adsorption active sites, leading to greater methy­
lene blue adsorption. The results show that high void volume and pore
connectivity are critical to ensure high adsorption values(Novais et al.,
2018b). In addition, the results show that the porous geopolymer
spheres, as shown in Fig. 15, enabled faster adsorption equilibria (20%
shorter time for equilibria) and higher methylene blue absorption (a
twofold increase) compared to other geopolymers shapes reported to
date, due to their larger geometric surface area per unit volume(Novais
et al., 2019). Spherical samples (diameter = 2.6 mm) provided better
results than cylindrical discs (thickness = 3 mm; diameter = 22 mm) for
wastewater purification(Novais et al., 2018b, 2019). On the other hand,
Shao et al. (2020) demonstrated that in large-scale wastewater treat­
ment, a zeolite/geopolymer composite membrane, as shown in Fig. 16,
is better performing under actual working conditions. This study also
provides an effective concept for improving the foam adsorption per­
formance by adding a second phase, such as zeolite(Alothman, 2012;
Pimraksa et al., 2020; Rożek et al., 2019, 2020), activated carbon(Chen
et al., 2020b), carbon nanotubes(Wabaidur et al., 2020), metallic oxides
(Chen et al., 2019; Wang et al., 2020), silica and lignocellulosic additives
(Chen et al., 2020b), hydrotalcite(Papa et al., 2019), etc. And the adding
functional additives to the fly ash-based porous geopolymer was well
addressed in previous work(Zhang et al., 2021).

Table 3
Maximum heavy metals and dyes adsorption capacity of various fly ash-based porous geopolymer reported in the literature.
Refs Adsorbate Adsorbent C0 (ppm) T (C) pH qmax (mg/ Removal efficiency Equilibrium time
g) (%) (h)

Duan et al. (2016) Cu2+ Bulk (1–5 g/L) 100–200 40 6 113.4 n.r. 3
Novais et al. (2016d) Pb2+ Cylindrical disc (d = 22 mm; h = 3 mm) 50 RT 5 6.3 n.r. 24
Onutai et al. (2019) Pb2+ Fiber (0.1 g) 20 25 5 n.r. ~83 n.r.
Onutai et al. (2019) Cd2+ Fiber (0.1 g) 20 25 5 n.r. ~24 n.r.
Onutai et al. (2019) Cu2+ Fiber (0.1 g) 20 25 5 n.r. ~33 n.r.
Onutai et al. (2019) Ni2+ Fiber (0.1 g) 20 25 5 n.r. ~13.5 n.r.
Han et al. (2020) Pb2+ Bulk (15*15*15 mm) 1150 60 4 123.2 n.r. 60
Kaewmee et al. Ca2+ Bulk(20 g/L) 125 RT 8.3 37.6 n.r. 6
(2021)
Kaewmee et al. Mg2+ Bulk(20 g/L) 125 RT 8.3 26.1 n.r. 24
(2021)
2+
Tan et al. (2021) Ni Spheres (1–3 spheres) 200–2000 RT 2–6 19.94 41.06 48
Liu et al. (2016) MB Powder n.r. 25 n.r. 50.7 98 48
Novais et al. (2018b) MB Cylindrical disc (d = 22 mm; h = 3 mm) 1–50 RT 5.9–9.6 15.4(1st) 64.8(1st) 30
109.6(6th) 48.4(6th)
Novais et al. (2019) MB Spheres 10–250 RT 5.6–10 30.1(1st) 90.3(1st) 26
79.7(6th) 84.6(9th)
Shao et al. (2020) MB ANA/GP membrane 100 RT n.r. 95 40(15th) 1.5
Kaewmee et al. MB Cube (1–5 g/L) 10–1000 RT n.r. 84.6(1st) n.r. 6
(2020)
Nurddin et al. (2020) MB Spheres (3.5 g/L) 350 RT n.r. n.r. 85.37 n.r.

Refs = References; n.r. = not report; RT = Room temperature; MB = Methylene blue.

14
X. Li et al. Journal of Cleaner Production 359 (2022) 132043

Fig. 14. EDS map of fly ash-based porous geopolymer after (a) Pb2+ (Novais et al., 2016d) (Reproduced with permission from Journal of Hazardous Materials;
published by Elsevier) and (b, c) methylene blue (Novais et al., 2018b, 2019) ( (Reproduced with permission from Journal of Cleaner Production; published by
Elsevier) adsorption tests; (d) Maximum heavy metal and dye adsorption capacity of various fly ash-based porous geopolymers reported in the literature.

Fig. 15. Optical images of the initial (a) and after MB adsorption with various concentration ((b) 10, (c) 25, (d) 75, (e) 100, (f) 175 and (g) 200 ppm) of FA-based
geopolymer spheres with real colors; Influence of MB initial concentration(h) and the number of regeneration cycles (i) on the uptake and removal efficiency of MB
by FA-based porous geopolymer spheres(Novais et al., 2019). (Reproduced with permission from Journal of Cleaner Production; published by Elsevier).

It is worth noting that fly ash-based geopolymer foam adsorbents can
be recovered and reused. At present, only two reports have studied the
recovery and reuse performance of fly ash-based geopolymer foams. The
FA-0.57 sample prepared by Novais et al. was recycled for 5 times and,
in the fifth cycle, the absorption and removal efficiency of methylene
blue changed only slightly, which clearly demonstrates the possibility of
reusing this innovative adsorbent without affecting performance(Novais
et al., 2018b). Porous geopolymer spheres displayed superior perfor­
mance. At the end of eight cycles, the spheres maintain their integrity (as
observed by SEM) and, more importantly, in the eighth loop the removal
efficiency was higher than 83%, and more cycles led to a cumulative
high uptake (79.7 mg/g), which is more than that reported for all other
geopolymer adsorbents in powder form(Novais et al., 2019).
3.7. pH control
After a geopolymer is solidified, the free alkali remaining in the
geopolymer framework easily diffuse to the surface and react with
carbon dioxide in the atmosphere to form a white carbonate deposit
(weathering). Studies have shown that, for porous fly ash-based geo­
polymer samples, a larger pore size distribution and higher total
porosity will lead to faster alkali leaching, which leads to faster

15
X. Li et al.
weathering(Zhang et al., 2014). This feature may reduce its durability as
a structural material in applications such as reinforced concrete, but it is
very advantageous for applications such as wastewater treatment,
anaerobic digestion and other biological processes, as well as those
having pH requirements to ensure high efficiency. In 2010, Lloyd et al.
(2010) analyzed the solution extracted from hardened fly ash-based
geopolymers, confirming that the pore network of these materials is
rich in alkali metal cations and that the solution pH was >13. In
anaerobic digestion, when the pH is less than 6.6 the efficiency of the
reactor will significantly decrease, and as fly ash-based porous geo­
polymers slowly release free alkali into an aqueous medium, they ensure
that the pH value is maintained, thereby creating a passive pH control
system.
Previous studies have shown that the leaching rate of fly ash-based
porous geopolymers is affected by the SiO2/Na2O and SiO2/Al2O ra­
tios(Bumanis and Bajare, 2014), their open porosity (Bumanis and
Bajare, 2014; Novais et al., 2016c) and the liquid-solid ratio(Novais
et al., 2016c). The leaching of alkali into water is mainly affected by the
SiO2/Na2O and SiO2/Al2O ratios. By changing the molar ratios of the
components, materials with different buffer capacities can be obtained.
A high SiO2/Na2O ratio can ensure the maximum leaching of the alkali
into the solution, while an increase of Al2O3 content limits the leaching
of alkali due to the trapping effect of the Al ion going into fourfold co­
ordination. Second, open porosity is another factor affecting the leach­
ing effect. A highly porous structure can ensure the gradual leaching of
alkali over a long period of time(Bumanis and Bajare, 2014). Adding
glass powder to the raw material can increase the rate of alkali leaching
by 19–32% because the glass frit has a material composition with a
higher SiO2/Na2O content, and the particle size and physical properties
16
Journal of Cleaner Production 359 (2022) 132043
Fig. 16. (a) Rejection and water permeability rates of
the ZM@SCS composite membrane for various
organic wastewaters and the GPM@SCS for MB; (b)
Cyclic filtration performance of the ZM@SCS for
removal MB solution; Digital (inset of (b)) and SEM
images of the ZM@SCS with top-view (c) and cross-
section view (d) after 15 times of cycles; (e) Pro­
posed filtration mechanism diagram for the removal
of organic pollutants using the ANA-ZM@SCS. (GPM
= Geopolymer membrane; RhB=Rhodamine B;
CR=Congo red; TC = Tetracycline; p-NP = p-nitro­
phenol; OTCC=Oxytetracycline; GP = Geopolymer,
SCS=Porous sintered sand core slice, ANA = Anal­
cime; ZM = Zeolite membrane; ZM@SCS= Porous
sintered sand core slice supported zeolite membrane;
GPM@SCS= Porous sintered sand core slice sup­
ported geopolymer membrane) (Shao et al., 2020).
(Reproduced with permission from Journal of Haz­
ardous Materials; published by Elsevier).
of the base glass powder also affect the rate of leaching(Bumanis et al.,
2015). Varying the solid-to-liquid ratio to adjust the leaching rate of fly
ash may also be controlled using the geopolymer matrix to reduce the
solid-liquid ratio of OH− ions to promote faster and more complete
leaching. However, this widens the pH gradient and weakens the geo­
polymer pH buffering capacity, so by controlling the solid-liquid ratio, a
fly ash-based porous geopolymer with a narrow range of pH fluctuations
can be obtained, increasing its potential as a pH buffering agent(Novais
et al., 2016c). Novais et al. (2017) synthesized fly ash-based porous
geopolymer spheres(Fig. 17). These innovative spheres, which can be
easily handled, improve the simplicity and efficiency of the process, and
have a higher specific surface area that enhances the alkali release
ability. The fly ash spheres show the lowest pH fluctuation (1.6–1.9) and
a higher maximum alkali leaching capacity (0.0317 mol/dm3g).
Although the above studies indicate the potential use of fly ash-based
porous geopolymers as pH buffers, previous studies have been carried
out in distilled water, and few studies have been carried out under more
severe actual conditions. Novais et al. (2017) evaluated the use of their
porous spheres to control the pH in the anaerobic digestion of cheese
whey (substrate), which has high acidity. When they first operated
without the spheres in the reactor, the pH was stabilized mainly between
a value of 3.84 and 4.38, thus inhibiting the production of methane.
However, when the spheres were added the pH value was mostly
maintained within the values of 6.45 and 7.94, which is conducive to the
early and continuous generation of methane (lasting for 70 days), and
the methane content in the biogas was as high as 78%(Novais et al.,
2018c).
X. Li et al.
Fig. 17. SEM images of spheres(a); Cumulative leaching amount of OH− ions(b) and the leaching percentage (inset of (b)) and pH variation (c) with time for
geopolymer spheres without FA content and with various FA content (33-75 wt%) (Novais et al., 2017). ( Reproduced with permission from Journal of Cleaner
Production; published by Elsevier)
4. Summary and future prospects
Porous geopolymers have the advantages both in terms of processing
(low energy consumption, low pollution, low cost) and of characteristics
(low thermal conductivity, good thermal stability and unique adsorption
behavior). Porous geopolymers prepared from fly ash as the main min­
eral raw material can also address the problem of environmental
pollution caused by it, since it is a hazardous solid waste. Fly ash-based
porous geopolymers can be employed for thermal insulation in build­
ings, sound insulation, pH buffers, and water softening agents, and can
also be applied to sewage treatment as adsorbents, realizing the concept
of “waste control by waste”. Therefore, manufacturing fly ash-based
porous geopolymers with excellent performance is a very important
opportunity; however, some problems remain to be solved before they
can be widely implemented.
(1) At present, the main method of preparing fly ash-based porous
geopolymers is the direct foaming method, which introduces a
foaming agent into the system, and a variety of foaming agents
have been developed to prepare these components. The type of
foaming agent directly determines the pore structure character­
istics and affects the properties, and therefore their overall effect
and their influencing mechanisms deserve further, more
comprehensive studies. In fact, because of the different compo­
sitions of the fly ash and of the geopolymer matrix, and the
different specific technological processes and curing conditions
used in the various studies, a direct and straightforward com­
parison is currently not feasible.
(2) In the sacrificial template method, the use of PVA templates and
the heat treatment and alkali treatment adopted in the removal
have increased the cost of materials to a certain extent, which will
cause environmental pollution and waste resources. Moreover,
the removal difficulty of the template is greatly increased in
large-scale applications. Developing a template with lower cost
and less difficult to remove is a promising trend for future
research on the sacrificial template method.
17
Journal of Cleaner Production 359 (2022) 132043
(3) The excellent thermal insulation, high temperature resistance,
flame retarding ability and sound insulation characteristics of fly
ash-based porous geopolymers indicate their potential use as
building materials. However, it is worth noting that the realiza­
tion of components possessing low thermal conductivity and a
high sound absorption coefficient mostly depends on the pres­
ence of a large volume of porosity, which carries with it a sig­
nificant reduction in strength, limiting their use in the field of
building materials to some extent. Therefore, it is very important
to develop fly ash-based porous geopolymers taking both aspects,
high porosity and sufficient strength, into account. Possibly,
introducing a certain amount of a lightweight material into the
system could provide a way to solve this problem.
(4) The adsorption of heavy metal ions and organic dyes by fly ash-
based porous geopolymers is quite significant. Although not
much research on this aspect is available, it also confirms their
potential application in wastewater treatment. In particular, fly
ash-based porous geopolymer microspheres prepared by the
suspension curing method greatly expand the contact area with
the adsorbate, improving its adsorption efficiency, can easily
generate an adsorption bed and can easily be recycled. However,
to be applied to sewage treatment in practice, we must first solve
the problem of treating the adsorbents after adsorption. Secondly,
concerning organic dyes, the adsorption behavior of the material
has been so far confirmed only for methylene blue, and the
adsorption of other organic dyes has not been demonstrated.
Finally, although some studies have explained the adsorption
mechanism by fitting adsorption kinetic curves and isothermal
adsorption curves, further studies are needed to explain the se­
lective adsorption and the reasons for the different adsorption
characteristics of different adsorbates from the perspective of
mechanism. Furthermore, the use of geopolymers for adsorbing
anionic pollutants should be also explored and, since in this case
the ion exchange between cations would not occur, other
adsorption mechanisms should therefore be investigated and
validated.
X. Li et al.
Declaration of competing interest
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.
Acknowledgements
This work was supported by National Natural Science Foundation of
China [52002090]; Heilongjiang Postdoctoral Science Foundation
Funded Project (LBH-Z19051), the Fundamental Research Funds for the
Central Universities (3072021CF1021; 3072021CF1003), and the Sci­
entific Research Foundation for the Returned Overseas Chinese Scholars
of Heilongjiang Province (2019QD0002).
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