1

Introduction to geopolymers
J L Provis and J S J van Deventer,
University of Melbourne, Australia

Abstract: This introductory chapter provides a brief overview of some

important aspects of geopolymer technology, in particular its historical
development and the terminology by which geopolymers are described.
An introduction to geopolymer technology from a scientific viewpoint is
also given. The scope of this review is confined to predominantly low-
calcium materials, i.e. ‘traditional’ alkali-aluminosilicate geopolymers, to
the exclusion of alkali-activated slags and other related materials.

Key words: geopolymer, inorganic polymer, aluminosilicate, alkali

activation.

1.1 History of geopolymer technology

The term ‘geopolymer’ was coined in the 1970s by the French scientist and
engineer Prof. Joseph Davidovits, and applied to a class of solid materials
synthesised by the reaction of an aluminosilicate powder with an alkaline
solution (Davidovits 1982a, 1991, 2008). These materials were originally
developed as a fire-resistant alternative to organic thermosetting polymers
following a series of fires in Europe, and products based on this initial work
have since found application as coatings for fire protection for cruise ships
(Talling 2002), as a resin in high-temperature carbon-fibre composites (Lyon
et al. 1997), in thermal protection of wooden structures (Giancaspro et al.
2006), as a heat-resistant adhesive (Bell et al. 2005, Krivenko and Kovalchuk
2007), as a monolithic refractory (Comrie and Kriven 2003, Kriven et al.
2004), and in various other niche applications. However, as can be seen from
a brief perusal of the Table of Contents of this book, the primary application
for geopolymer binders has since shifted to uses in construction. This is
primarily due to the observation, first published by Wastiels et al. (1993),
that it is possible to generate reliable, high-performance geopolymers by
alkaline activation of fly ash, a by-product of coal combustion.
The synthesis of construction materials by alkaline activation of solid,
non-Portland cement precursors (usually high-calcium metallurgical slags)
was first demonstrated by Purdon (1940). Detailed lists of key historical
references and milestones in the development of alkali-activated binders
have been presented in various review papers (Malone et al. 1985, Krivenko
1994, Roy 1999, Krivenko 2002); the majority of these relate to the alkaline

1
2 Geopolymers

activation of blast furnace slags, and so are beyond the scope of the current
discussion. A very extensive review focussed predominantly on alkali activation
of metallurgical slags has recently been published (Shi et al. 2006), and the
reader is referred to that excellent book for information in that area. The key
distinction to be made here is that the alkaline activation of slags produces
a fundamentally calcium silicate hydrate-based gel (Richardson et al. 1994,
Wang and Scrivener 1995, Shi et al. 2006), with silicon present mainly in one-
dimensional chains and some substitution of Al for Si and Mg for Ca, whereas
the geopolymer gel is a three-dimensional alkali aluminosilicate framework
structure (Duxson et al. 2007b). The role of calcium in geopolymers is a
matter still under investigation; some of the subtleties of calcium chemistry
in geopolymers will be discussed throughout this book.
Much of the early published research into aluminosilicate geopolymers
was published in the patent literature (for example: Davidovits 1982b,
1984), and so contains little scientific detail. Probably the most valuable
documents summarising work throughout the 1980s are the proceedings
of a conference (Geopolymer ’88) held in France in 1988 (Davidovits and
Orlinski 1988), and a review paper authored by Davidovits (1991). Shortly
after this, Palomo and Glasser published the first detailed scientific study
of metakaolin geopolymers (Palomo and Glasser 1992), followed shortly
afterwards by an extremely valuable three-part series by Rahier et al. (1996a,
1996b, 1997). These papers laid the groundwork for both broader and
deeper study of metakaolin geopolymers in the ensuing decade, in particular
work by groups in Spain (Granizo and Blanco 1998, Palomo et al. 1999b,
Alonso and Palomo 2001), New Zealand (Barbosa et al. 2000, Barbosa and
MacKenzie 2003), Germany (Kaps and Buchwald 2002, Buchwald et al.
2003, Buchwald 2006), and Australia (Yip and van Deventer 2003, Duxson et
al. 2005, Perera et al. 2005, Singh et al. 2005, Steveson and Sagoe-Crentsil
2005). The proceedings of Geopolymer conferences held in 1999 (Davidovits
et al. 1999), 2002 (Lukey 2002) and 2005 (Davidovits 2005) also provide
valuable information regarding both technical developments in the field and
the worldwide growth in geopolymers research during this period. A book
published recently by Davidovits (2008) also summarises a good deal of
work that was only previously available in the patent literature.
Research into fly ash geopolymers has grown from the aforementioned
conference paper by Wastiels et al. (1993) to now form the bulk of
applications-oriented research in this field. Fly ash has long been used in
Portland cement concretes to enhance flow and other properties (Diamond
1986, Bouzoubaâ et al. 1999, Manz 1999), to reduce the carbon footprint
of concrete, as well as simply a means of disposing of some of the many
millions of tonnes of fly ash produced worldwide each year. Additional
early reports of geopolymerisation of ASTM Class F (low-calcium) fly ash
were provided by a number of researchers (van Jaarsveld et al. 1997, 1998,
 Introduction to geopolymers 3

Palomo et al. 1999a, van Jaarsveld 2000, Krivenko and Kovalchuk 2002,
Lee and van Deventer 2002, Swanepoel and Strydom 2002, Fernández-
Jiménez and Palomo 2003, Rostami and Brendley 2003, Hardjito et al. 2004,
Palomo et al. 2004), along with a proliferation of patents. Possibly due to
the inherent difficulty associated with detailed scientific analysis of highly
heterogeneous fly ash-based geopolymers, the level of understanding of fly
ash geopolymers currently appears to lag behind their metakaolin-based
counterparts. Metakaolin geopolymers are often used as a ‘model system’
by which the more commercially relevant fly ash-based materials may be
better understood (van Deventer et al. 2007), and the exact degree to which
this relationship holds has been the subject of some recent scrutiny (Lloyd
2008).
It is also necessary to note that various theories have been proposed
attempting to link aspects of geopolymerisation technology to the construction
of ancient structures, most particularly the Pyramids of Egypt (Davidovits
and Davidovits 2001, Barsoum et al. 2006). While the veracity of such
arguments is still under quite intense debate in some circles, it is clear that
whether or not the Pyramids were ‘poured’ as synthetic stone blocks, the
chemistry involved in such an undertaking would have been some distance
away from the alkali-activated aluminosilicate systems which today are
described as geopolymers (Barsoum et al. 2006). However, it is not the role
of this Introduction to attempt to speculate regarding such issues.

1.2 Geopolymer terminology

In the context of this book, a ‘geopolymer’ is in general defined as a solid
and stable aluminosilicate material formed by alkali hydroxide or alkali
silicate activation of a precursor that is usually (but not always) supplied
as a solid powder. The same term has also been used to describe organic
polymers formed under geological conditions (e.g., coal); in spite of some
highly speculative discussions to the contrary (Davidovits 2008), these
materials are entirely unrelated to aluminosilicate geopolymers and will not
be discussed in detail here.
The materials referred to here as ‘geopolymers’ have also been described
in the academic literature as ‘mineral polymers’, ‘inorganic polymers’,
‘inorganic polymer glasses’, ‘alkali-bonded ceramics’, ‘alkali ash material’,
‘soil cements’, ‘hydroceramics’, and a variety of other names. The major
impact of this proliferation of different names for essentially the same material
is that researchers who are not intimately familiar with the field will either
become rapidly confused about which terms refer to which specific materials,
or they will remain unaware of important research that does not appear upon
conducting a simple keyword search on an academic search engine. A prime
example of this is the very valuable early work of Rahier and colleagues
4 Geopolymers

(Rahier et al. 1996a, 1996b, 1997), who used the term ‘inorganic polymer
glass’ rather than ‘geopolymer,’ and so these papers have received far fewer
citations than their quality and importance deserve. The terms ‘geopolymer’
and ‘inorganic polymer’ are gaining increasing ubiquity in the academic
research field, and will be used essentially interchangeably throughout this
book. Geopolymers are a subset of the broader class of alkali-activated
binders (Shi et al. 2006), which also includes materials formed by alkali-,
silicate-, carbonate- or sulfate-activation of metallurgical slags and giving
a product that is predominantly calcium silicate hydrate, as mentioned in
Section 1.1. The defining characteristic of a geopolymer is that the binding
phase comprises an alkali aluminosilicate gel, with aluminium and silicon
linked in a three-dimensional tetrahedral gel framework that is relatively
resistant to dissolution in water (MacKenzie 2003, Rees et al. 2007).
More than 25 years ago, Davidovits introduced the ‘sialate’ nomenclature
to describe aluminosilicate structures (Davidovits 1982a). The linkage
type Si-O-Al was named a sialate bond, and Si-O-Si a siloxo bond. This
provided a means of describing the composition of geopolymers according
to their Si/Al ratio, with a ratio of 1.0 being a poly(sialate), 2.0 being a
poly(sialate-siloxo), and 3.0 a poly(sialate-disiloxo). Unfortunately, the term
‘sialate’ was already in use (since the 1950s) to describe any of the salts of
sialic acid, a nine-carbon monosaccharide and an important component of
several biochemical systems within the human body. Also, this system of
nomenclature implies certain aspects of the geopolymer gel structure which
do not correspond to reality; firstly, it describes only integer Si/Al ratios, and
secondly, it provides a one-dimensional description of a three-dimensional
network, which will almost invariably prove inadequate. This nomenclature
system did for some time find relatively widespread use in academic research
(Barbosa et al. 2000, Zoulgami et al. 2002, Zhang et al. 2005, Subaer and
van Riessen 2007), often to describe systems with non-integer Si/Al ratios
but generally without comment as to its applicability in such cases, but
appears to be fading in popularity as researchers discover its limitations.

1.3 Geopolymer science

Given that a large part of the purpose of this book is to provide an overview
of the state of the art in various aspects of geopolymer science, it would be
superfluous to provide a detailed description in this Introduction. Nonetheless,
some preliminary comments are in order.
Initially, it must be said that geopolymers are a complex class of materials.
The principal means of synthesising geopolymers is to combine an alkaline
solution with a reactive aluminosilicate powder, in particular metakaolin
(calcined kaolinite clay) or fly ash (a by-product of coal combustion). This
results in the formation of a disordered alkali aluminosilicate gel phase,
 Introduction to geopolymers 5

known as the geopolymeric gel binder phase. Embedded within this phase
are unreacted solid precursor particles, and the pore network of the gel
contains the water that was used in mixing the precursors (usually supplied
via the alkaline ‘activating solution’). Unlike in a calcium silicate hydrate
gel, the water does not form an integral part of the chemical structure of a
geopolymer binder; from a practical perspective this presents both advantages
and disadvantages. The fundamental framework of the gel is a highly
connected three-dimensional network of aluminate and silicate tetrahedra,
with the negative charge due to Al3+ in four-fold coordination localised on
one or more of the bridging oxygens in each aluminate tetrahedron and
balanced by the alkali metal cations provided by the activating solution.
There have been a variety of attempts to draw schematic diagrams of the
three-dimensional geopolymer structure; such efforts will almost certainly
be fraught with difficulty due to the disorder inherent in the geopolymer and
also the difficulty of accurately representing a three-dimensional framework
in two dimensions. The picture presented recently by Rowles et al. (2007)
is probably the most useful of those currently available.
It has also been shown that the geopolymeric gel binder displays structural
similarities, on an atomic to nanometre length scale, to zeolitic materials.
In some cases – particularly in the presence of high water content, elevated
synthesis temperature and low Si/Al ratio – this extends so far as to be
visible as the formation of nanocrystallites within the geopolymer gel (Provis
et al. 2005). However, even where none of these factors is present and the
geopolymer displays no structural ordering on a length scale exceeding 1
nm, there are still strong structural motifs on an atomic length scale which
correlate well with those observed in zeolites (Bell et al. 2008).
From this basis, the structural analysis presented in various chapters of
this book represents the results of detailed investigations by various research
groups over a number of years. Very little about the structural analysis of
geopolymers is straightforward, as they comprise a mixture of various X-ray
amorphous phases (reaction product as well as unreacted precursor material),
and are formed in a corrosive reaction environment which complicates in situ
analysis (as discussed in detail in Chapter 4). Nonetheless, much information
has been obtained through careful experimental design and data analysis. In
most areas of science, it is the case that either ‘easy’ (i.e. routine) methods
of analysis are applied to ‘challenging’ materials, or ‘challenging’ methods
of analysis are applied to ‘easy’ (i.e., pure and well characterised) material
classes. Geopolymers, in common with Portland cements, are a ‘challenging’
class of materials whose chemistry necessitates the use of ‘challenging’
techniques for characterisation; this means that the science involved in
understanding ‘low-technology’ construction materials is in fact at the cutting
edge of materials science in general.
6 Geopolymers

1.4 Geopolymer applications

As was mentioned in Section 1.1, the primary area of application of geopolymer
technology is currently in the development of reduced-CO­2 construction
materials as an alternative to Portland-based (calcium silicate) cements.
Various other properties of geopolymers provide technological advantages
over traditional construction materials, but performance in itself will not be
sufficient to drive a revolutionary change in construction materials technology
(Duxson et al. 2007a). A new material cannot be forced onto an unwilling
market; the market itself must demand a new material, and this is beginning
to be the case for geopolymers in construction, as will be discussed in detail
in Chapter 17 of this book.
Other applications for geopolymers include as a host matrix in waste
encapsulation, as a low-cost ceramic (either used directly or as a precursor
for calcination), and in fire protection of structures. Part III of this book is
dedicated to the description of some of the prime applications for geopolymers
at present.

1.5 Conclusions
Geopolymers are a class of materials, whose potential remains to be fully
unlocked. It is only through a detailed understanding of geopolymer science
that full use can be made of the properties of geopolymers in specific
applications. However, such science would rapidly become irrelevant in
the absence of commercial success; a material that is well characterised but
not used in the real world is in effect useless. From a scientific perspective,
debates regarding nomenclature and semantics are entirely counterproductive,
so long as the existing nomenclature is adequate to the task at hand. What is
more important is that the understanding of geopolymers is built to the point
where binder properties can be tailored a priori by rational mix design, and
the understanding of the binder structure is sufficient to explain why these
properties can be expected to last for a sufficient period of time to render
the material fit for purpose in an engineering sense.
There is a growing demand for new construction materials that have low
greenhouse gas emissions associated with their manufacture. Therefore,
geopolymeric concrete could potentially be used widely as a replacement for
Portland cement concrete, but this will only happen when both an efficient
supply chain for raw materials and a distribution network for the products
are in place. Recent commercial initiatives in this regard are encouraging,
but it will take some time to make geopolymeric concrete a scaleable
commodity available on a global basis. In the meantime, it is imperative
that the localised demonstration of geopolymer technology grows, especially
for converting coal ash into concrete with a low carbon footprint. This book
 Introduction to geopolymers 7

provides essential background to those interested in pursuing this exciting

technology.

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 Introduction to geopolymers 9

Lloyd, R. R. (2008) PhD Thesis, Department of Chemical and Biomolecular Engineering,

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10 Geopolymers

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