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Geopolymerization and Its Potential Application in Mine

Tailings Consolidation: A Review
a a
Feng Rao & Qi Liu
a
Department of Chemical and Materials Engineering, University of Alberta, Edmonton,
Alberta, Canada
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 Mineral Processing & Extractive Metall. Rev., 36: 399409, 2015
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ISSN: 0882-7508 print/1547-7401 online
DOI: 10.1080/08827508.2015.1055625

Geopolymerization and Its Potential Application in

Mine Tailings Consolidation: A Review
FENG RAO1 and QI LIU
Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, Canada

A new class of construction materials has been in development in the past several decades through geopolymerization reactions
of aluminosilicate minerals, which can potentially replace ordinary Portland cement (OPC). In this paper, the brief history
Downloaded by [University of Alberta] at 08:27 17 July 2015

of the development of the geopolymerization technology was reviewed with particular emphasis on the differences between
conventional geopolymers, alkali-activated metallurgical slags, and zeolites. Studies on both the raw materials and the
alkali activators in the geopolymerization processes were also reviewed. As oil sands tailings and many mine tailings contain
aluminosilicate minerals as their main constituents, geopolymerization reactions have been explored as a potential technological
route to treat these tailings for tailings consolidation and heavy metal xation.
Keywords: aluminosilicate minerals, consolidation, geopolymer, metal xation, reclamation, tailings

1. Geopolymers and Geopolymerization
1.1. Geopolymers and Their Development
Geopolymers are aluminosilicate materials with three-
dimensional (3D) amorphous micro-structures. They are
formed by geopolymerization processes in which the oxides
of silicon and aluminum minerals or aluminosilicate
minerals are activated by alkalis to form 3D polymeric chains
(Provis and van Deventer 2009). Although Glukhovsky and
Krivenko used alkali activated metallurgical slag in construc-
tion in 1950s (Glukhovsky 1994), and even some ancient
structures, like the Pyramids in Egypt, are believed to be
products of geopolymerization (Barsoum et al. 2006), the
terms geopolymer and geopolymerization were rst of geopolymer gel is usually compared with the synthesis of
coined by Davidovits in 1972 (Davidovits 1999) and in the
1980s (Davidovits 1982), respectively. Table 1 presents
a summary of the major historical references and milestones
in the development of geopolymers. In the past 30 years,
the applications of geopolymers have been expanded from
its original use as re-resistant materials, to alternative
construction materials and stabilizers for solid wastes.
The raw materials for synthesizing geopolymers have
also been widened from metakaolin and y ash to various
aluminosilicate minerals, clays, solid wastes, and their
mixtures.
1
Currently with Universidad Michoacana de San Nicolas de
Hidalgo, Mexico.
Address correspondence to Qi Liu, Department of Chemical
and Materials Engineering, University of Alberta, Edmonton,
AL T6G 2V4, Canada. E-mail: qi.liu@ualberta.ca
Color versions of one or more of the gures in this article
can be found online at www.tandfonline.com/gmpr.
For instance, alkali-activated metallurgical slags are con-
sidered geopolymers (Shi et al. 2006). However, the alkali-
activated metallurgical slags differ from the conventional
geopolymers in that: (1) the precursor materials for alkali-
activated slags are rich in calcium so that calcium silicate
hydrate (CSH) gels are the main reaction products, whereas
the precursor materials for the conventional geopolymers
are low in calcium and rich in silicate and aluminum, so that
in conventional geopolymers amorphous aluminosilicate
networks are formed. (2) The silicon in CSH gels exists
mainly in one dimensional chains, whereas geopolymer
gel is a three-dimensional alkali aluminosilicate network
(Duxson et al. 2007; Li et al. 2010). In addition, the synthesis
zeolite, because both involve the formation of zeolite
precursor: tetrahedral silicon (SiOH4  ) and tetrahedral
aluminum (AlOH4  ). However, these zeolite precursors
form an amorphous microstructure in geopolymers while
they form the crystalline microstructure in zeolites (Criado
et al. 2007; Komnitsas and Zaharaki 2007).
Geopolymers have been considered as a replacement
of ordinary Portland cement (OPC) in construction industry
because it shows comparable cementitious properties, but
the production of geopolymers leads to approximately
80% lower CO2 emissions (Provis et al. 2007). However,
unlike the intensive scientic research on the synthesis and
characterization of geopolymers, much less progress
has been made in the industry to accept geopolymers as
construction materials. Researchers attributed this to the
fact that performance in geopolymer alone cannot drive
a revolutionary change in construction materials (Davidovits
2008; Duxson et al. 2007a; van Deventer et al. 2012).
Appropriate infrastructure and ecosystem also need to be
developed to enable the transition.
 400 F. Rao and Q. Liu

Table 1. Summary of geopolymer development with highlights of the applications in treating mineral and oil sands processing
tailings
Author Year Description Signicance

Glukhovsky 1950s Alkali activated slag with products of both CSH and Aluminosilicate hydrate was found and
& Krivenko aluminosilicate hydrate was used in construction used
Davidovits 1972 A new technical language for the transfer of basic The term geopolymer was coined
scientic information
Davidovits & 1988 Proceedings of geopolymer-rst European conference Summarizing works on geopolymer
Orlinski on soft mineralurgy throughout the 1980s
Wastiels et al. 1993 Mineral polymer based on y ash First report of geopolymers by alkaline
activation of y ash
Rahier et al. 1996a, Low temperature synthesized aluminosilicate glasses Groundwork for both broad and deep
1996b, study of metakaolin geopolymers
1997
Xu and van 2000, 2002 Geopolymerization of multiple minerals Geopolymerization of alumino-silicate
Deventer wastes, extending precursors from
metakaolin and y ash
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Duxson et al. 2007 The review paper Geopolymer technology: the extensively reviewed the developments of
current state of the art geopolymers
Davidovits 2008 The book geopolymer chemistry & applications
2nd edition
Provis and 2009 The book Geopolymers: structure, processing,
van properties and industrial applications
Deventer

Geopolymerization is an integrated process for the
synthesis of geopolymers, which involves leaching, diffusion,
reorientation, polymerization and condensation (Komnitsas
and Zaharaki 2007). Figure 1 shows a schematic diagram
of the geopolymerization process. In the rst stage of
geopolymerization, aluminate and silicate tetrahedral
monomers are generated by alkali dissolution of solid
aluminosilicate precursors. In the second stage, the mono-
mers form oligomers which lead to the dissolution of more
precursor materials, so that the solution is saturated
with a complex mixture of silicate, aluminate and alumino-
silicate species, which polymerize into an amorphous gel.
This gel is then condensed and hardened into geopolymers.
The mechanical performance of the geopolymers is
evaluated by exural strength and compressive strength.
Microstructures of the geopolymers were studied by X-ray
diffraction (XRD), scanning electron microscope (SEM),
nuclear magnetic resonance (NMR), and so on (Provis and
van Deventer 2009).
Most investigations directly correlated the geopolymer
performance with the precursor materials such as the type
of aluminosilicates, the Si and Al ratio in the aluminosili-
cates, and the type and concentration of alkali activators
(Khale and Chaudhary 2007). Some studies analyzed more
fundamentally the formation of geopolymer gel and the nal
geopolymer concrete, for instance the effects of silica and
alumina release rate (Hajimohammadi et al. 2010), the geo-
polymer gel development, the transformation of geopolymer

Fig. 1. Schematic diagram of the geopolymerization process. Early research focused more on the correlation between geopolymer
performance and leaching (van Jaarsveld et al. 2002). Recent investigations focused more on the details of geopolymer formation
mechanisms (Rees et al. 2007).
 Geopolymerization and Its Potential Application in Mine Tailings Consolidation
gel into nal geopolymer concrete (Fernandez-Jimenez et al.
2006b) and the heterogeneity of geopolymer concrete in
geopolymerization (Rees et al. 2007; van Deventer et al.
2007). These topics remain interesting and require further
studies. Researchers have also contributed intensive work
to introducing geopolymers into commercial applications
(van Deventer et al. 2010, 2012).
1.2. Raw Aluminosilicate Materials and Alkali Activators
Metakaolin was initially used as the raw material and has
become a model compound in geopolymerizaion, usually
used to compare with other precursor materials, for instance
y ash (Davidovits et al. 1991). A number of other raw mate-
rials, including natural minerals, metallurgical wastes and
their mixtures, were exploited to synthesize geopolymers in
recent years. Diaz-Loya et al. (2011) studied the mechanical
properties of 25 y ash-based geopolymers from different
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sources. They reported that the mechanical behavior of these
geopolymer cements were similar to that of OPC concrete.
Xu and van Deventer (2000) used 16 natural minerals,
which were classied into four crystal structure groups
(ortho-, di- and ring-silicates, chain silicates, sheet silicates,
and framework silicates) and six mineral groups (garnet,
mica, feldspar, clay, sodalite, and zeolite), to synthesize
geopolymers. They found that natural aluminosilicate
minerals could be a source material for geopolymers, and
the framework aluminosilicates show a higher extent of
Fig. 2. Geopolymers synthesized from (A) y ash, (B) kaolinite and y ash, (C) albite, kaolinite and y ash (Xu and van
Deventer 2003).
401
dissolution in alkaline solution, thus a higher compressive
strength after geopolymerization, than the chain, sheet and
ring structure aluminosilicates.
As reported in the literature, the raw aluminosilicate
materials in geopolymerization can be broadly divided into
two groups: (1) calcined materials such as y ash, metakao-
linite, slag, construction residues and pozzolanic wastes; (2)
noncalcined materials such as kaolinite, feldspar, clays, and
mineral processing tailings. Geopolymerization of calcined
raw materials generally has faster dissolution and gelation
rate that results in geopolymers which show higher early
compressive strength than non-calcined materails. This
phenomenon was attributed to the fact that calcination
improves the reactivity of the raw materials by changing
the crystalline structure into an amorphous structure that
is easier to leach. However, geopolymers synthesized from
non-calcined raw materials display a higher increase in the
compressive strength in the later stage of the geopolymeriza-
tion reaction. And geopolymers synthesized from a mixture
of calcined and non-calcied materials benet from the inter-
action between the raw materials that could activate each
other and enhance the extent of the reaction to generate a
high compressive strength product (Xu and van Deventer
2002, 2003). Figure 2 shows a series of SEM images of
geopolymers (together with their compressive strength)
synthesized from three types: namely y ash, y ash and
kaolinite, y ash, kaolinite and albite, at optimal mass ratios.
A thicker gel phase can be observed from geopolymers
 402
synthesized with y ash and kaolinite than those synthesized
from y ash alone. With the addition of albite, more y ash
particles were transferred to the gel phase, so that fewer large
y ash particles are observed in the image. The nal
compressive strength of the three geopolymers follows the
order: GPy ash < GPy ashkaolinite < GPy ashkaolinitealbite. they used y ash together with kaolinite and albite as the
In addition, the two main structural elements of geopoly-
mers (Si and Al) and their ratio in raw materials play
a critical role in geopolymerization, and have been studied
extensively. Davidovits proposed geopolymer structure
as a sialate (silicon-oxo-aluminate) network consisting of
SiO4 and AlO4 tetrahedras linked alternately by sharing all
oxygen atoms. Cations such as Na, K, and Ca2 are present
in the framework cavities to balance the negative charge of
SiO4 and AlO4 (Figure 3). Their empirical formula is

SiO2=Al2O3 ratio for compressive strength development of
Mn SiO2 z  AlO2  wH2 O 1
n metakaolinite geopolymers was in the range of 3.43.8, and
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where M is the alkaline element, z is 1, 2, or 3 representing the
structures of polysialate (-Si-O-Al-O-), polysialate-siloxo
(Si-O-Al-O-Si-O) and polysialate-disiloxo (Si-O-Al-O-Si-O-
Si-O), respectively, and n is the degree of geopolymerization
(Davidovits 1982; Singh et al. 2005). Table 2 presents some
typical geopolymers synthesized with various SiO2=Al2O3
ratios. In this table, although the listed values of compressive
strengths at different SiO2=Al2O3 ratios cannot be compared
with each other because the geopolymers were synthesized by
different researchers under different conditions, these values
do suggest that geopolymers can be synthesized by using a
wide range of SiO2=Al2O3 ratios (from 1.6 to 5). Van Deventer
Fig. 3. The sialate geopolymer structure proposed by
Davidovits (1982).
F. Rao and Q. Liu
and his colleagues used a relatively low SiO2=Al2O3 ratio to
synthesize y ash-geopolymers, which can be attributed to
the intrinsic properties of their y ashes used in Australia
(Phair et al. 2004; Phair and van Deventer 2001; van Jaarsveld
et al. 2002). They reported a higher SiO2=Al2O3 ratio when
raw materials (Xu and van Deventer 2003). Because the
formula for kaolinite is 2SiO2Al2O3  2H2O (or a deduced for-
mula of metakaolinite, 2SiO2Al2O3) (Bergaya and Lagaly
2013), the geopolymers synthesized with metakaolinite should
possess a SiO2=Al2O3 ratio higher than 2. Furthermore, silica
or quartz is the main impurity in kaolinite, and silicate is
a common activator in geopolymerization, so that SiO2=Al2O3
ratios higher than 2.5 were usually reported in literature
(Cheng and Chiu 2003; Puertas 2000; Rowles and OConnor
2003; Silva 2007). Some researchers stated that the optimal
increasing the SiO2=Al2O3 ratio from 3.8 to 5.0 leads to
a decrease of the compressive strength (Rowles and OConnor
2003; Silva 2007; Stevenson and Sagoe-Crentsil 2005).
Therefore, while Davidovits and his co-workers consider
that the SiO2=Al2O3 ratio in geopolymers should be between
1 and 3, representing the three sialates (Figure 3), the other
researchers advanced this hypothesis and developed
geopolymers with a SiO2=Al2O3 ratio of higher than 3. For
instance, polysialate-trisiloxo (Si-O-Si-O-Al-O-Si-O-Si-O),
might also exist in a geopolymer structure.
Alkali activator signicantly affects the geopolymeriza-
tion on leaching silicon and aluminum from raw materials
and on the formation of aluminosilicate glassy gel, as
well as on the condensation process. The alkali activators
can be divided into two categories, namely alkalis such
as NaOH, KOH, Na2CO3 and K2CO3 and silicate additives
such as Na2SiO3 and K2SiO3 (Duxson et al. 2007;
Fernandez-Jimenez et al. 2013; Xiong et al. 2004). Table 3
summarizes some experiences for controlling alkali activa-
tors from various research groups. Although different
designs were reported, it can be concluded that alkali activa-
tors usually consists a very high alkali concentration and an
optimal silicate additive. In most studies, the high alkali
concentrations were expressed as weight ratios with respect
to the raw materials, for example, metakaolinite and y
ash, or as stoichiometric concentration in the precursor
solutions. For instance, Wang et al. (2005) reported that
the exural strength, compressive strength and apparent
density of metakaolinite geopolymer increased with increas-
ing NaOH concentration from 4 mol=L to 14 mol=L. They
attributed this increase to the enhanced dissolution of the
metakaolinite particulates at high-alkali concentrations.
The effect of pH of the precursor slurry on the mechanical
properties of synthesized geopolymers has also been
reported. Phair and van Deventer (2001) synthesized y
ash based geopolymers and stated that the compressive
strength at pH 14 was 50 times higher than that at pH 12.
They observed that the geopolymer precursors remained
viscous and behaved like cement at lower pH, and attained
a more uid gel composition at higher pH, which was less
viscous and more workable. They found that more small
 Geopolymerization and Its Potential Application in Mine Tailings Consolidation 403
Table 2. Typical geopolymers synthesized with different Si=Al ratios

Curing in Oven
Compressive
SiO2= Alkali Temp Time Additives strength
Reference Al2O3 Metal ( C) (h) Main raw material (mass%) (MPa)

van Jaarsveld et al. (2002) 1.75 K 30 24 Fly ash Kaolinite (15%) 51.4
Phair et al. (2004) 1.67 Na 23 Fly ash Kaolinite (14%) 32.7
Phair et al. (2001) 1.64 Na 45 24 Fly ash Cement (12%) 50
Xu and van Deventer (2003) 2.10 K 40 24 Kaolinite, y ash 45
and albite
Xu and van Deventer (2003) 2.30 K&Na 40 24 Kaolinite and 24.4
albite
Cheng and Chiu (2003) 3.13 K 60 3 Blast furnace slag Metakaolin 79
Rowles and OConnor 2.6 Na 75 24 Metakaolinite 15
(2003)
Puertas et al. (2000) 3.33 Na 65 1.25 Kaolinite 54
Silva et al. (2007) 3.81 Na 40 24 Metakaolinite 23
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Silva et al. (2007) 5.01 Na 40 8 Metakaolinite 18

silicate oligomers and monomers were formed at higher properties of the geopolymers (Figure 4). However, Fernandez-
slurry pH (Phair et al. 2000). In general, researchers agreed Jimenez and Palomo (2005a) reported from an alkali activation
that a higher alkali concentration prompted the geopolymer- of a y ash geopolymer that increasing Na2O from 14.1 wt%
ization reactions, and thus resulted in better mechanical to 14.9 wt% led to a reduction of the mechanical properties,

Table 3. Typical experiments on designing alkali activators

Reference Raw materials Activating solution Optimal activator Curing detail

Rahier et al. (1997) Metakaolinite: 85% SiO2=Na2O: Constant SiO2=Na2O: 1.4 60 C for 24 hours
Non-reactive minerals: at 1.4 H2O= Na2O: 11.9
15% H2O= Na2O: 8.913.9 Sodium silicate=
Sodium silicate= metakaolinite: 1.0
metakaolinite:
0.81.7
Liew et al. (2012) Metakaolin NaOH: 610 mol=L NaOH: 8 mol=L 80 C for 7 days
SiO2: 54% SiO2=NaOH: 0.160.28 SiO2=NaOH: 0.2
Al2O3: 31.7%
Wang et al. (2005) Metakaolinite NaOH: 412 mol=L NaOH: 12 mol=L 65 C for 10 hours
Si: 42.39% NaOH=Na2SiO3: NaOH=Na2SiO3:
Al: 29.86% 4.15:1 4.15:1
O: 26.17%
Phair and van Deventer Metakaolin pH: 1214 pH: 14 45 C for 24 hours
(2001) Slag Al2O3= SiO2: 6.16.4 K-silicate and KOH
Fly ash
Fernandez-Jimenez and Fly ash Na2O: 5%15%a Na2O: 14.09%a 85 C for 20 hours
Palomo (2006b) SiO2: 53.1% SiO2: 09.52%a SiO2=Na2O: 0.118
Al2O3: 24.8%
Ma et al. (2012) Fly ash Na2O: 1%1.5%a Na2O: 1.5%a 40 C for 28 days
SiO2: 48.4% SiO2: 01.5%a SiO2: 1%a
Al2O3: 31.4%
Bakharev (2005) Fly ash Na2O: 28% Na2O: 8% 75 C for 28 days
SiO2: 50% SiO2=Na2O: Constante SiO2=Na2O: 2.02
Al2O3: 28% at 2.02
Rattanasak and Fly ash NaOH: 515 mol=L NaOH: 15 mol=L 65 C for 48 hours
Chindaprasirt (2009) SiO2: 39.5 SiO2=NaOH: 0.5-2 SiO2=NaOH: 1 Separate mixing of
Al2O3: 19.5% NaOH and
SiO2.
a
Weight percent in the y ash and alkali activator mixtures.
 404
Fig. 4. A comparison of the reported effects of alkali
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concentrations on the compressive strength.
although the reason was not clear. The effect of alkali
concentration on the geopolymers mechanical properties
and the leaching or catalytic mechanism is still an interesting
area that can be studied further. However, this effect should
be studied together with the cation and anion type of the
alkalis and the addition of silicate. For instance, carbonate
ion can form sodium bicarbonate that decreases the degree
of geopolymerization when carbonate alkalis are utilized
(Fernandez-Jimenez and Palomo 2005b).
As soluble silicate additive is widely used and studied in
geopolymerization, the silicate to alkali ratio (SiO2=M2O)
is a synthesizing parameter in many studies. It is reported
that the structural stability of geopolymers increased with
the addition of silicates, a result due to the formation of long
chain silicate oligomers as well as Al-O-Si complexes in the
geopolymeric gels (Lee and van Deventer 2002; McCormick
et al. 1989). However, recent studies show that the addition
of soluble silicate does not induce fundamental changes in
the structure of the produced geopolymer. Neither XRD
nor NMR studies indicated a change of the sample from
amorphous to crystalline when the soluble silicate concen-
tration was increased (Duxson et al. 2005a; Khale and
Chaudhary 2007; Provis et al. 2005). Furthermore, Criado
et al. (2007) found from an FTIR study on the formation
of y ash geopolymers that a high-soluble silicate concen-
tration (2%) promotes the formation of Si-rich gels with a
higher percentage of bridge bonds and results in a more
amorphous system, although a low concentration of mono-
meric soluble silicate is known to promote the formation of
network tectosilicate geopolymers. Cheng and Chin (2003)
found that excess silicate hinders water evaporation, and
thus impedes geopolymeric structure formation. Therefore,
it is important to design an optimal soluble silicate dosage
in the synthesis of geopolymers, which should be considered
with respect to other conditions such as the raw material
type and the alkalinity.
The Na and K are the main cations in geopolymer
systems, possibly because sodium hydroxide and potassium
F. Rao and Q. Liu
hydroxide are the most widely used alkalis. These cations
have been studied extensively and they play the charge bal-
ancing role in the formation of tetrahedral silicon
(SiOH4  ) and tetrahedral aluminum (AlOH4  ), and in
the condensation of geopolymer gel. However, conicting
results were reported when comparing the effects of Na
and K. Fernandez-Jimenez et al. (2013, 2006a) reported
that Na has a greater capacity than K to accelerate the
setting and hardening reactions in y ash geopolymerization
when all the other conditions are kept the same, and thus the
sodium geopolymers had higher mechanical strength than
potassium geopolymers. Based on the results of strength
measurements and SEM and MAS NMR analyses, they
attributed the observed differences to a balance of two
opposing mechanisms: (1) the higher alkalinity of the potass-
ium salts, which induces higher aluminosilicate solubility
than sodium salts and (2) the smaller ionic radii of Na,
which gives the sodium ion a higher charge density than
K. The Na ions can thus link the formed silicate and
aluminate monomers more effectively for the crystallization
of pre-zeolitic gel, while K favors the formation of larger
and looser silicate oligomers. However, while Fernandez-
Jimenez et al. (2013, 2006a) considered the smaller ionic
radii of Na ions as the main contributing factor for the
higher mechanical strength of sodium geopolymer, van
Deventer et al. (Duxson et al., 2005b; van Jaarsveld and
van Deventer 1999a) emphasized the higher alkalinity
of potassium salt as the main contributing factor, and they
stated that although potassium geopolymers (y ash) have
higher porosity and a lower degree of crystallinity, they show
higher compressive strengths than sodium geopolymers.
They explained this effect further by employing 2H, 27Al
and 23Na MAS NMR techniques to observe the structural
properties and mechanism of (AlOH4  ) formation in
metakaolin-based geopolymers. They reported a higher
conversion from Al(V) and Al(VI) to Al(IV) at a higher
K=Na ratio after synthesizing fteen geopolymers.
1.3. Other Factors Affecting Geopolymerization
Beside the raw starting materials and alkali activators, many
other factors also play an important role in geopolymeriza-
tion. For instance, mechanical activation has been tested as
an effective means to improve the reactivity of y ash in geo-
polymerization (Kumar et al. 2007). Temuujin et al. (2009)
reported that grinding y ash in a vibration mill with a mill-
ing media to powder ratio of 10:1 led to an 80% increase in
compressive strength of the produced geopolymers when
compared with geopolymers synthesized from raw material.
Another study stated that (1) vibratory mill shows superior-
ity over other mills on inducing reactivity, and (2) the y ash
reactivity varies non-linearly with median particle size in
mechanical activation (Kumar and Kumar 2011). And as
shown in Tables 2 and 3, the curing time and curing tem-
perature are very different, resulting in different compressive
strengths of the geopolymers even with similar raw materials
and activator. Muniz-Villarreal et al. (2011) reported that
the optimum curing temperature was 60 C for a metakaolin
geopolymer after investigating temperatures of 30, 40, 50,
 Geopolymerization and Its Potential Application in Mine Tailings Consolidation
60, 75 and 90 C. Furthermore, the water content in the geo-
polymerization process varied widely, and the ratio of water
to silicate in raw materials (H2O=SiO2) or the ratio of water
to alkali activators (H2O=M2O) were tested as geopolymer
synthesizing parameters. Interested readers can refer to the
excellent reviews by Khale and Chaudhary (2007) and
Komnitsas and Zaharaki (2007) for the effects of those
parameters on geopolymerization.
2. Research on Using Geopolymers to Consolidate
Mine Tailings
Mine tailings generally contain process water, gangue miner-
als, heavy metals and any toxic substances used in the dress-
ing of the ores. They are usually disposed of into tailings
ponds in slurry form. The disposal of mine tailings is a major
environmental liability, and is becoming more serious with
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the increasing mining activities for metals that need to work
on lower-grade and more complex ores. Mine tailings could
cause serious water pollution, arising from the discharge of
water contaminated with solids, heavy metals, mill reagents,
sulfur compounds, etc. Even worse, failure of steep-sided
tailing dams can happen due to earthquakes, blasting
vibration and extreme weather (Wills and Napier-Munn
2006). Therefore, backll technology, and the use of mine
tailings as road paving materials and construction bricks
have been exploited (e.g., Mahmood and Mulligan 2007;
Zou and Li 1999). Backll or tailings re-use as construction
materials requires the consolidation and strengthening of the
tailings slurry, especially when it consists of ne particles
that are difcult to settle. Therefore, geopolymerization
process has been employed as a technology to stabilize and
strengthen mine tailings. In the geopolymerization process,
the silicon and aluminum-rich mine tailings were suitable
raw materials. Similarly, geopolymerization reactions were
exploited to stabilize or consolidate industrial slag and soil
from civil construction that contain required raw materials
for geopolymers. Ogundiran et al. (2013) reported that up
to 10% y ash could be replaced by lead smelting slag in
the synthesizing process of y ash based geopolymers, which
had the potential of producing stabilizers for lead smelting
slag. Zhang et al. (2013) found that metakaolinite based
geopolymers were effective soil stabilizer for clayey soils in
civil engineering constructions.
Davidovits (1987, 1993) pointed out that geopolymer
cement could be used to stabilize mine tailings. Sand, mine
tailings and geopolymers in the ratio of 20:13:7 were blended
to produce solidied tailings. Tailings from four different
types of mines, base metal, potash, coal and uranium mines,
respectively, were tested. After casting, setting and curing at
ambient temperatures, the solidied products were tested for
resistance to leaching. Davidovits concluded that the
geopolymer-stabilized-and-solidied mine tailings had
archaeological long-term stability. Xu and van Deventer
(2002) studied the geopolymerization of different minerals,
and their results suggest that a wide range of Al-Si based
minerals could be used as source geopolymerization precur-
sors. Geopolymerization could result in the immobilization
405
of toxic metals by geopolymeric binders due to physical
encapsulation and chemical bonding (van Jaarsveld et al.
1999b). van Jaarsveld et al. (2000) reported that geopolymer-
ization was used to stabilize one mine tailings with satisfac-
tory compressive strength and durability, as well as low
permeability, using between 60 and 75% of mine tailings as
the main ingredient. Pacheco-Torgal et al. (2007, 2008)
synthesized tungsten mine tailings based geopolymer as a
cementitious material with high early stage strength. They
evaluated different new binders and showed the feasibility
to utilize tungsten mine tailings as construction materials
by geopolymerization. However, their process involved a
thermal treatment step at 950 C for 2h, which renders the
process unattractive from an environmental perspective.
Zhang et al. (2011) and Ahmari et al. (2012a) utilized dry
copper mine tailings, y ash and activator solutions to
synthesize geopolymer pastes. Based on the results of SEM
imaging, XRD analysis and unconned compressive
strength tests, they concluded that mine tailings, with
addition of y ash from 0 to 75%, were a viable and prom-
ising construction material if the geopolymerization process
was applied. They investigated the formation of geopolymer-
based bricks at an elevated temperature (optimal 90 C) by
using the copper mine tailings as the main raw materials.
Their results showed that copper mine tailings can be used
to produce eco-friendly bricks based on the geopolymeriza-
tion technology to meet the ASTM standards. Interestingly,
the compressive strength and durability of the tailings bricks
were signicantly enhanced when cement kiln dust (CKD)
was added (Ahmari et al. 2012b, 2013a, 2013b). In addition,
Jiao et al. (2013) utilized stone coal tailings from vanadium
extraction to synthesize thermally stable geopolymers. They
found that dry ball milling could enhance the dissolution
reaction and promote the geopolymerization process. These
studies reveal the possibility to apply geopolymerization
process to stabilize and utilize mine tailings. However, no
study reported a geopolymerization process that uses 100%
mine tailings as the raw materials. Additives, such as y
ash and=or metakaolinite, were used in all geopolymerization
processes studied thus far to consolidating mine tailings.
3. Potential Application of Geopolymerization to
Consolidate Oil Sands Tailings
In a typical mine tailings pond, the coarse particles settle
quickly, form a mud bottom and a layer of aqueous suspen-
sions containing dissolved metal ions and suspended ne
particles (Figure 5). Comparatively, the Alberta oil sands
tailings ponds contain higher percentages of suspended ne
solids and clays together with residual bitumen, which form
the non-settling mature ne tailings (MFT) with a solids
content of 3040 wt% and a residual bitumen content
around 1 wt% (Rao and Liu 2013). The main components
in the solid fraction are silt and clays, which are composed
of 4070 wt% kaolinite, 3045 wt% illlite and 10 wt% mixed
layer illite=smectite (BGC Engineering Inc. 2010). The
accumulation of MFT in oil sands tailings ponds poses
severe environmental issues such as long-term containment,
 406
Fig. 5. Photos of typical mine tailings (A) (Ground truth trekking, 2012) and Alberta oil sands tailings (B) (Tar sands solution
(TSS) network, 2013).
delayed reclamation, sterilization of oil sands resources.
Downloaded by [University of Alberta] at 08:27 17 July 2015
They are also a major threat to migratory birds and to the
ecosystem in northern Alberta. However, current technolo-
gies on consolidating the oil sands tailings have focused
almost exclusively on removing water from the settled tail-
ings sludgea difcult task in oil sands industryand there
is currently no known commercial technology to make con-
solidated stackable oil sands tailings. The geopolymerization
technology can potentially be used to strengthen the oil
sands tailings leading to their consolidation (Esmaeili et al.
2012). On the basis of the reaction mechanisms of geopoly-
merization process, a number of reasons would support this
prospect:
1. Source materials: although the residual bitumen might
be detrimental for the geopolymerization process, the
majority of the ne solids in oil sands tailings are kaolinite
and illite with minor quantities of smectites and illite-
smectite. The tailings also contain large quantities of silica
sands (Mikula et al. 1996). The sands and clays, rich in Si
and Al, are excellent source materials for geopolymerization.
2. Activators: the compressive strength requirement for oil
sands tailings sludge and the time period to reach the
compressive strength are signicantly lower than those
geopolymers used in other areas. Therefore, there is a
possibility that the geopolymerization of oil sands tailings
sludge could start at a weak alkaline solution and high
water=solid ratio. The oil sands tailings have a natural
pH between 8 and 9, which provides a good starting point
for activation of geopolymerization reactions.
3. Water chemistry of recycle process water after geopoly-
merization: considering that the addition of an activator,
for example, sodium hydroxide or potassium hydroxide,
is required for geopolymerization of oil sand tailings, there
might be an accumulation of sodium or potassium ions
in the recycle water. Also the pH of the recycle water
may be higher than that commonly used in industrial
oil sands extraction. However, the change of water
chemistry of recycle water is not expected to adversely
inuence bitumen recovery. Systematic studies from
Masliyah and other researchers indicated that (1) higher
pH (up to 11.8) is favorable to bitumen liberation from
sand grains; and (2) no direct correlation between the
F. Rao and Q. Liu
concentration of monovalent metal ions (Na and K)
and bitumen recovery was observed (Masliyah et al. 2004).
4. Research Opportunities
4.1. Mechanism of Geopolymerization
The geopolymerization of aluminosilicates involves very
different construction materials chemistry and synthesis
pathways compared with the CSH chemistry that underpins
OPC. Thus the fundamental mechanism of geopolymeriza-
tion need to be well understood. Although intensive investi-
gations on the synthesis and characterization of geopolymers
have been carried out, it is obvious to notice the lack of
understandings on the geopolymerization reaction mech-
anism and synthesizing parameters. More research should
be focused on the geopolymerization mechanisms and the
formation of standards or well repeatable parameters in
synthesizing geopolymers, to address the following questions
1. Is an amorphous structure of the raw material, induced
by calcination, necessary to increase dissolution and
enhance geopolymerization?
2. A systematic study on the factors impacting geopolymeric
pre-cursors formation. These factors include the type
(structure) of raw materials, the type of activators, water
contents, Al and Si contents, calcination, curing tempera-
ture and time, and so on.
3. The correlation between the degree of geopolymeric
structures formed in geopolymerization process and the
nal mechanical performance of the geopolymers.
4. As many research followed the sialate geopolymer
structure proposed by Davidovits, it is reasonable to
study more deeply into the structural factors of Si and
Al respectively in the geopolymers and the adhesion
structure between the geopolymer and non-reacted
raw minerals, as well as the differences and similarities
between geopolymer and zeolite.
4.2. Geopolymerization to Stabilize Mine Tailings and
Oil Sands Tailings
1. Based on the understanding of the mechanisms of geopo-
lymerization, studies on consolidating mine tailings can
 Geopolymerization and Its Potential Application in Mine Tailings Consolidation
be carried out. The ability of geopolymerization on
immobilizing heavy metals and the inuence of sulfur
on geopolymerization should be studied.
2. Similarly, oil sands extraction tailings may be consoli-
dated by geopolymerzation. The types and dosages of
activators, the compressive strength of the resulting
treated tailings as a function of curing time, curing
temperature using these activators need to be established.
The effect of oil sands tailings composition on the
compressive strength of the Geopolymerization-treated
tailings should be studied, and the effect of organics
(bitumen and polymer occulants) on the geopolymeriza-
tion reactions should be investigated.
5. Conclusions
A review of literature revealed the potentials of using
Downloaded by [University of Alberta] at 08:27 17 July 2015
geopolymerization reactions in consolidating and strength-
ening mine and oil sands tailings as these tailings typically
contain the required aluminosilicate source materials. The
open literature also showed conicting reports in the geopo-
lymerization processes regarding for instance the suitable
Si=Al ratios, the function of metal cations such as sodium
and potassium, and the effect of calcination. Although
a high activator concentration results in better mechanical
properties of the synthesized geopolymers, a long reaction
time, which would typically be allowed in mine tailings
treatment, may also improve the mechanical properties of
the treated mine tailings thus allowing the use of lower alkali
activator dosages. Therefore, the potential applications of
geopolymerization on consolidating mine tailings and oil
sands extraction tailings seemed a worthwhile prospect.
Systematic studies should focus both on the fundamental
geopolymerization mechanisms, such as reaction pathways,
structurestrength correlations, and on the various process
parameters on the geopolymerization of mine tailings, parti-
cularly the Alberta oil sands tailings, as the latter is currently
the most acute problems in the Alberta oil sands operations.
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