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 December 2013
VOL. 65 NO. 12

Surface mining equipment

Sustainable energy in mines
Rare earths in China

Special Editorial Supplement: Tunneling & Underground Construction

[Link]
 Technical Papers

Geopolymer-based concrete
to reduce carbon footprint of
the construction industry
by H. Akbari, T. Heller, S. Shin, X. Yang, P. Kolay, S. Kumar and M.K. Mohanty

Abstract n Ordinary portland cement (OPC) is the key pozzalonic component of the concrete
mix widely used as a construction material worldwide. Billions of tons of OPC are used in the
construction industry each year. However, calcinations of limestone and silica that produce
OPC also produce almost an equal amount of CO2 during the cement manufacturing process.
Thus, OPC production accounts for nearly 7% of all anthropogenic CO2 emissions each year.
The main objective of this study was to develop a geopolymer-based composite to be used as
a substitute for OPC in concrete application to significantly lower the carbon footprint of the
construction industry. A waste material produced during the coal combustion process was used
as the main raw material for the geopolymer-based composite. It was mostly the nonmetallic
content of the F-type fly ash produced from the combustion of bituminous coal. The authors
envisioned extracting some of the valuable metal oxides from fly ash prior to using the major
nonmetallic portion of the fly ash for geopolymer concrete application. The results obtained from
this study showed that the compressive strength of geopolymer concrete compares favorably
with that of conventional concrete prepared using OPC.

Mining Engineering, 2013, Vol. 65, No. 12, pp. 57-62.

Official publication of the Society for Mining, Metallurgy and Exploration, Inc.

Introduction of the calcination process and com- in conventional concrete.

The portland cement industry is bustion of fossil fuels. The amount of Joseph Davidovits introduced a
known to have a significantly large car- CO2 produced by chemical processes three-dimensional alumino-silicate
bon footprint, as it causes about 7% in cement plants is the second largest complex with a very strong binder net-
of the total CO2 emissions worldwide industrial source of CO2 emissions in work of Al and Si elements, which he
(IPCC, 2005). During the production the United States (EPA, 2010). CO 2 named “geopolymer” because the raw
of one ton of ordinary portland ce- emissions from cement production in- materials are inorganic (Davidovits,
ment (OPC), about 1 t (1.1 st) of CO2 creased by 24% during the period 1990 1988). This new material is the result of
is released to the environment because to 2008. As a majority of the scientific a polymerization process using Al- and
community believes that global warm- Si-rich materials with alkaline metals, as
ing is caused by emission of greenhouse shown in Eq. (1).
H. Akbari, member SME, T. Heller, gases like CO2, there is a worldwide
S. Shin and X. Yang, member SME, effort to lower the emission of CO 2 Si − Al materials + activators
are graduate students and S. Kumar in the earth’s atmosphere. Several at- (NaOH, Na2SiO3, KOH) + H2O 
and M.K. Mohanty, member SME, tempts are in progress to reduce the geopolymer backbone + H2O (1)
professors at Southern Illinois consumption of OPC to lower the re-
University Carbondale, Carbondale, sulting CO2 emissions. These attempts The raw materials for producing
IL. Paper number TP-13-022. Original are comprised of two main areas: one geopolymer can be any high-Al or -Si
manuscript submitted April 2013. using supplementary materials to add material, including natural minerals
Revised manuscript accepted for to the concrete instead of cement; e.g., such as kaolinite and clays and byprod-
publication August 2013. Discussion coal combustion byproducts such as fly uct materials such as fly ash, bottom
of this peer-reviewed and approved ash, bottom ash and boiler’s slag. The ash, blast furnace slag, rice-husk, red
paper is invited and must be other is to find other types of binders mud, etc. Choosing the kind of raw ma-
submitted to SME Publications by for concrete (Rangan, 2008). This paper terial in the geopolymerization process
March 31, 2014. is about a different type of binder mate- depends on availability, cost, type of ap-
rial suitable for playing the role of OPC plication, specific demand of the end
[Link] Mınıng engıneerıng DECEMBER 2013 57
users and so on. It has been observed by several research- Over the last few decades, the concrete industry has given
ers that geopolymers have perfect mechanical properties, as special attention to the safe and economical utilization of
well as fire and acid resistance. So, during the past 20 years, these CCBs (Helmuth, 1987). Current research on the ben-
these new materials have been looked into as a very suitable eficial use of CCBs in building and highway construction
substitution for the OPC for concrete applications in the has identified several promising uses for these materials. In
building and construction industries (Xu and Van Deventer, addition to use in concrete, CCBs have been successfully
2000). With regard to climate change and greenhouse gas used in the agricultural industry, blasting grit and roofing
emissions, geopolymers could effectively decrease the CO2 material, cement clinker making, flowable fill, grout, mineral
emission released by cement plants. Some advantages of filler, mining applications, snow and ice control, wallboard,
geopolymers are: roller compacted concrete, structural fill, embankments and
soil stabilization (Kalyoncu, 2003). Several case histories of
• Waste consumption: the geopolymer concrete basi- utilization of coal combustion byproducts in construction
cally can be made of waste products such as fly ash, projects are available (ACAA, 2008; GAI, 1988; Golden,
bottom ash, furnace slag, red mud, etc. 1986; Korcak, 1998; Kumar and Stewart, 2003a and b; Lovell
• Reduction of CO2 emissions: they could reduce the et al., 1997; Naik et. al., 1997; Schroeder, 1994; Seals et al.,
demand for OPC so the CO2 production resulting 1972; Tikalsky and Carrasquillo, 1989).
from OPC manufacturing will be decreased. Balaguru et al. (1999) reported success in using geopoly-
• Reduction in the use of natural resources: geopoly- mer concrete to increase the compressive strength of rein-
mer uses waste material, whereas OPC uses natural forced concrete beams. Moreover, a good performance of fire
resources. resistance and durability was observed. Palomo et al. (2004)
• Reduced need of space for disposal of waste materi- presented excellent performance of fly ash-based geopoly-
als. mer concrete in the production of railway sleepers. Hardjito
• Less water consumption: in the geopolymerization and Rangan (2005) carried out research on low-calcium fly
process, water plays a minor role, while in the mak- ash-based geopolymer concrete. They investigated several
ing of OPC, the hydration role of water is very im- variables affecting the geopolymerization process and short-
portant. term properties of geopolymer concrete. Wallah and Rangan
• Geopolymer composite has high resistance to fire (2006) investigated the long-term properties of low calcium
and corrosion. fly ash-based geopolymer concrete, e.g., creep behavior under
sustained load, drying shrinkage behavior, sulfate resistance
Like any new technology, geopolymer technology has and resistance to sulfuric acid.
some challenges before it can be used in commercial appli- Some of the applications of geopolymers have been
cations. One of the challenges is the conservative nature of proved worldwide and implemented in building products,
the construction industry in accepting new materials. As this encapsulation of toxic metals, high temperature ceramic com-
technology is new, there is limited data about the durability posites and foundry applications (Komnitsas and Zaharaki,
of geopolymers. Finally, the performance of geopolymer con- 2007). Diaz et al. (2010) presented the results of their study
crete is measured by using standards developed for cement about producing geopolymer concrete with five different
concrete, which means there is a lack of standard methods for U.S. fly ash samples. They investigated some variables and
geopolymer materials (Duxson et al., 2007). suggested that a new definition is needed for class C and
The coal and utility industries are the major source of F fly ash as a raw material for geopolymer concrete. Some
mining and industrial wastes in the USA. The abundance of previous studies claimed that the low-calcium fly ash with
the coal resource and its use in electricity-generating plants loss on ignition (LOI) less than 5%, Fe2O3 less than 10% and
has resulted in the accumulation of large quantities of coal 80-90% particles smaller than 45 μm will produce a desir-
combustion byproducts (CCBs) over the last century. During able binder network of Si and Al (Fernandez-Jimenez et al.,
2008, about 123 Mt (136 million st) of CCBs were generated 2003). However, Van Jaarsveld et al. (2003) proved that any
in the U.S. by electric utilities and other sources (ACAA, increase in the amount of CaO in the fly ash will increase the
2008), and only 45% of total CCBs were put to use for ben- compressive strength of the concrete.
eficial applications (ACAA, 2008). The remaining CCBs are Past studies indicated that the CCBs obtained from the
disposed of in landfills and ash ponds. This has resulted in combustion of high sulfur coal contains 10% to 30% iron
the lack of available disposal space, high disposal costs and oxide, 15% to 30% Al2O3 and SiO2, 0.6% to 2% TiO2, 0.01%
environmental consequences for surrounding communities. to 0.1% MnO and other trace elements. Producing value-
In the 1920s, firing power plant boilers with pulverized added product has been an important aspect of reutilization
coal instead of lump coal was invented (WEPC, 2000). Cur- of CCBs. High-grade iron oxide extraction from CCBs, es-
rently about 75% of the boilers in the United States utilize pecially from coal fly ash, has been a promising concept. The
pulverized coal combustion systems (EPA, 1988). The pow- authors have developed a proprietary flowsheet to enrich the
dered coal is injected into a furnace with preheated air, where 17% iron oxide (by Davis tube measurement) in fly ash feed
it ignites and burns to completion while in suspension. Thus, to above 96% in the product (Mohanty et al., 2008). Many
most of the ash produced is very fine in size and remains in other researchers (for example, Honaker et al., 1997; Baird
suspension to be carried away by flue gases. This product is et al., 1998) were also able to successfully extract iron oxide
referred to as fly ash. The heavier ash, which sticks to the side from coal fly ash.
walls of the boilers and settles at the bottom of the furnace, One of the major resources of alumina is coal fly ash,
is known as bottom ash. whose industrial application has been limited because of
58 DECEMBER 2013 Mınıng engıneerıng [Link]
 Table 1
The analysis results of the SIPC fly ash samples.

Component Al2O3 SiO2 Fe2O3 CaO TiO2 Na2O K2O MgO S P2O5 L.O.I.
SIPC-XRF
14.90 38.50 26.70 3.69 1.01 0.91 3.33 1.04 2.30 0.62 7.00
analysis (%)

Table 2
The analysis results of the CWLP fly ash samples.

Component Al Si Fe Ca Ti Na K Mg V Zn Ni
CWLP-ICP
15.10 58.00 15.40 6.05 0.84 1.96 1.68 0.83 0.05 0.05 0.04
analysis (%)

high acid usage in the alumina extraction process. However, (CWLP) in Springfield, IL and Southern Illinois Power Co-
new methods, such as calcination of fly ash, combined with operative (SIPC) in Marion, IL, and brought to the Illinois
fresh fine coal and calcium oxide, have been developed dur- Coal Development Park, where a pilot-scale mineral pro-
ing past years to decrease the acid usage and increase the cessing facility is located. The X-ray fluorescence (XRF) and
alumina extraction efficiency (Bai et al., 2011). To increase inductively coupled plasma (ICP) analysis results of the two
the solubility of fly ash in acid solution, its crystalline mullite samples are listed in Tables 1 and 2. Clearly, the aluminum
·
phase (3Al2O3 2SiO2) should be destroyed by the sintering oxide and iron oxide contents in both ash samples are high.
process. Fly ash mixed with fresh fine coal (less than 1 mm The Davis tube tests showed that the magnetite content of
size) and calcium oxide is pelletized and calcinated at high the CWLP and SIPC fly ash samples are nearly 17% and
temperature to produce glassy phases like calcium silicate 10%, respectively.
and calcium aluminate, which have high solubility in acid.
Thereafter, the sintered fly ash is leached in sulfuric acid to Mineral extraction flowsheet design. The first step in
extract alumina. Finally, purification methods like solvent mineral extraction is a preconcentration step, primarily to
extraction, selective precipitation and crystallization are used separate iron oxide using a hydrocyclone. A Davis tube was
to separate the metal ions present in the solution from the used in the lab to separate the nonmagnetic fraction from
leaching process (Alquacil et al.,1987; Freeman, 1993; Harada the magnetic fraction to produce some feed material for the
et al., 1993; Matjie et al., 2005; Li et al., 2009; Bai et al., 2011). alumina extraction process. First of all, direct acid leaching
Titanium oxide is normally found in the form of rutile, without mullite decomposition on the fly ash sample was
anatase and brookite at relatively low grades. The extraction done. As indicated in recent literature (Bai et al., 2011), the
flowsheet varies depending on the individual ore charac- mullite phase of fly ash can be decomposed to increase the
teristics, but commonly consists of gravity separation, mag- Al extraction efficiency. Accordingly, the fly ash sample was
netic separation, froth flotation, hydrometallurgy and so mixed with fine clean coal (less than 1-mm size) and calcium
on. Researchers from China (Niu et al., 2010) have success- oxide in a mass ratio of [Link], respectively. Then, the new
fully upgraded low grade (4.5%) TiO2 to 47% (commercial mixture was pelletized into 4-9-mm spherical pellets and cal-
grade), which makes an extraction of TiO2 from CCBs appear cinated using a high temperature furnace at 900° C (1,652°
achievable. Other mineral extraction from CCBs has also F) for 150 min. The direct and sintered sample leaching tests
been rarely seen in literature. were done in 6.0 M sulfuric acid with a solid:liquid ratio of
High-sulfur coal fly ash (F-type) found in the midwest- 1:4 and in 80° C (176° F) temperature for 10 h. In each test,
ern U.S. is a Si-Al-rich material, making it a valuable raw the leachate was separated from the r esidual fly ash by filtra-
material for the geopolymerization process and production tion. The leached residue was washed using distilled water to
of geopolymer concrete after the extraction of the valuable remove the remaining leachate solution. Finally, the leached
metallic components. Introducing a successful geopolymer residue was dried in an oven at 80° C (176° F). Represen-
technology using coal fly ash will not only reduce significant tative samples from pregnant solution and leached fly ash
costs of disposing of fly ash in landfills and ash ponds and residues were collected and sent for analysis to determine
the associated environmental impacts, but will also result in the extraction efficiency for Al, Ti and Fe.
significantly reduced CO2 emissions due to the lower produc-
tion of OPC. In this study, two samples of midwestern coal Geopolymer-based concrete construction. In order to
fly ash were used to make geopolymer concrete samples and evaluate the suitability of high-sulfur coal fly ash for mak-
compare the compressive strength with that of traditional ing geopolymer concrete and its potential success as a con-
portland cement concrete. struction material, a preliminary study was conducted using
CWLP and SIPC fly-ash samples. There are about 10 param-
Materials and methods eters that affect the geopolymerization process and, thus, the
Sample collection and characterization. Two high-sul- characteristics of geopolymer concrete. The alkaline activator
fur coal fly ash samples were collected from two different was a combination of sodium silicate solution and sodium
power plant sites, the City Water, Light and Power company hydroxide or potassium hydroxide solutions (all commercial
[Link] Mınıng engıneerıng DECEMBER 2013 59
 Table 3
The new concrete composition for comparison of geopolymer and portland cement concretes.

Portland cement concrete Geopolymer concrete

Composition Composition
(kg) (%) (kg) (%)
Cement 5.635 13.7 Fly ash 5.635 13.9
Fine
Fine aggregate 13.862 33.6 13.862 34.3
aggregate
Coarse Coarse
18.455 44.7 18.455 45.7
aggregate aggregate
Water 3.321 8.0 Extra water 0.518 1.3
Total concrete 41.273 100.0 NaOH (16m) 0.986 2.4
Na2SiO3 0.986 2.4
Total
40.442 100.0
concrete

Figure 1 10 cm (4 in.) in diameter and 20 cm (8 in.) in height. The new

Geopolymer (cement-less) concrete samples made from the concrete composition is shown in Table 3.
fly ash samples.
Results and discussion
Mineral extraction. Using hydrocyclone preconcentra-
tion, the magnetite content of the SIPC fly ash sample was
enriched from 10% in the feed fly ash to 26.7% in the un-
derflow stream, with 92.7% recovery. It is believed that the
magnetite concentration can be enriched to about 35% by
further optimizing the process variables of the hydrocyclone.
A second cleaning step using a low intensity magnetic sepa-
rator would upgrade the Davis tube magnetite content >
96%. The nonmagnetic part of the fly ash sample was used to
further extract the valuable metals using direct and indirect
leaching tests. In the direct leaching test, the Al, Ti and Fe
extraction efficiencies obtained were 83%, 91% and 90%,
respectively. In the indirect leaching test, the results showed
that the Al, Ti and Fe extraction efficiencies were 82.7%,
86.2% and 89.6%, respectively. These results showed that
the ability of the leaching method to extract the Al, Ti and
the remaining part of the Fe is very high and more tests and
investigations are needed to optimize the process parameters.

Cement-less green concrete. Since geopolymer-based

grades). Several 5-cm (2-in.) cubes were prepared and tested concrete has as much as 80% less carbon footprint in com-
to obtain strength characteristics of geopolymer concrete parison to conventional portland cement-based concrete,
mortar prepared fly ash. The fly ash and fine aggregates in the the new term “green concrete” was coined by the research
mass ratio of 1:2.75 were mixed for 3 min. Then, the activa- group to refer to geopolymer-based concrete. Preliminary
tor consisting of sodium silicate solution (Na2O:14.7%, SiO2: tests were done to make geopolymer concrete using SIPC
27.4%, H2O: 55.9%), sodium hydroxide and extra water were and CWLP fly ash samples. Figure 1 shows the geopolymer
added to the dry mixture and mixed for 15 min. Samples were concrete samples made from high-sulfur coal fly ash samples.
then prepared and cured inside an oven and at room tem- To investigate the critical factors affecting geopolymer-
perature. After curing, the compressive strength tests were based concrete, a fractional factorial design was used to
performed. To compare the geopolymer concrete samples identify the critical process parameters. As illustrated by the
with the portland cement concrete, several 5-cm (2-in.) cubes half-normal probability plot of Fig. 2, alkali type (factor A)
of cement concrete were also prepared and tested to find the and concentration (factor B), curing temperature (factor E)
compressive strength of cement concrete samples. and H2O:Na2O ratio (factor D) have the most significant ef-
To further investigate and compare the geopolymer and fects on the compressive strength of the geopolymer concrete
cement concrete samples, a new composition of concrete samples made from fly ash. These four factors can be further
having coarse aggregate was used to make cylinder samples investigated to develop empirical models to predict the com-
60 DECEMBER 2013 Mınıng engıneerıng [Link]
 Figure 2 Figure 4
The comparative compressive strength data of the new
Factors having the most significant effect on the geopolymer concrete design results for geopolymer and cement.
concrete made from the SIPC fly ash sample.

increasing at the same rate as conventional cement concrete

did.
Figure 3 Conclusions
Cement and geopolymer concrete test results. This study envisioned a suitable processing scheme to
extract high-grade magnetite from fly ash generated from
burning high-sulfur coal. The leaching test done on the non-
magnetite part of SIPC fly ash samples showed that high
efficiency is achievable for Al, Ti and Fe extraction. In the
leaching tests, the extraction efficiencies of Al, Ti and Fe were
82.7%, 86.2% and 89.6%, respectively. These results showed
that the leaching process can effectively extract Al, Ti and Fe
from the nonmagnetite part of the Illinois fly ash. By con-
ducting statistically designed experiments, critical process
parameters affecting the compressive strength of geopoly-
mer-based concrete were identified. The results showed that
the alkali type and concentration, the curing temperature and
the H2O:Na2O ratio have the most significant effects on the
compressive strength of the geopolymer concrete samples
made from SIPC fly ash sample. The comparative compres-
sive strength data done on the new concrete composition
having fine and coarse aggregates indicated that the cement-
less concrete sample made by SIPC fly ash compared favor-
ably with that of the portland cement concrete. n

Acknowledgments
pressive strength achievable in the geopolymer concrete as a
The authors gratefully appreciate the funding for this
function of the critical process parameters.
study, which was provided by the United States Environmen-
Selected comparative compressive strength results ob-
tal Protection Agency.
tained by varying days of curing times are presented in Fig.
3. Clearly, the compressive strengths obtained from both fly
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