Ex Situ Mineral Carbonation

Environmental Science and Pollution Research (2021) 28:12202–12231
https://doi.org/10.1007/s11356-020-12049-4
REVIEW ARTICLE
A review on ex situ mineral carbonation

Shashikant Yadav 1 & Anurag Mehra 2
Received: 21 July 2020 / Accepted: 9 December 2020 / Published online: 6 January 2021
# The Author(s), under exclusive licence to Springer-Verlag GmbH, DE part of Springer Nature 2021
Abstract
The increased CO2 quantities in the environment have led to many harmful effects. Therefore, it is very important to decrease the
CO2 levels in the environment. CO2 capture along with safe and permanent storage using mineral CO2 sequestration method can
play an important role to reduce carbon emissions into the environment. Mineral sequestration is a stable storage method that
provides long-term storage and an appropriate substitute for the more popular geological storage method. The process is most
suited for places where there is a lack of underground cavities for underground geological storage. Minerals rich in Ca and Mg are
used predominantly in carbonation reactions. In addition, those alkaline wastes that are rich in Mg and Ca such as cement waste,
steel slag and many process ashes can also be employed in CO2 sequestration. Mineral carbonation could be used for the
sequestration of billions of tonnes of CO2 every year. However, various drawbacks related to mineral carbonation still need to
be addressed, such as resolving the slow rate of reactions, necessity of large amounts of feedstock, decreasing the high overall
cost of CO2 sequestration and reducing the huge energy requirements to accelerate the carbonation reaction. This study explores a
number of carbonation methods, parameters that control the process and future potential applications of carbonated products.
Keywords CO2 sequestration . Mineral carbonation . Waste stabilization . Waste utilization
Introduction stable carbonates (Owais et al. 2019; Neeraj 2020). The pro-
portion of Mg and Ca is about 2.0% and 2.1% of the total
Mineral sequestration is an important carbon sequestration Earth’s crust (Goff and Lackner 1998). Therefore, due to their
method, especially in areas where geological sequestration is abundance, minerals containing Mg and Ca are most suitable
not practicable due to underground leakage or non-availability raw materials for CO2 sequestration process (IPCC 2005).
of underground cavities (see Fig. 1) (Martín et al. 2018a; Li Forsterite (Mg2SiO4), a common magnesium silicate, for ex-
et al. 2019; Liu et al. 2019a; Pastero et al. 2019). Mineral ample, reacts with atmospheric CO2 and forms magnesium
sequestration is the safest method to provide sufficient capac- carbonate (MgCO3) (Huijgen and Comans 2003)
ity for sequestering maximum amount of the CO2 emission
Mg2 SiO4 ðsÞ þ 2CO2 ðgÞ→2MgCO3 ðsÞ þ SiO2 ðsÞ
(see Table 1) (Liu and Zhao 2000).
The basic idea of mineral sequestration is weathering, a Mineral carbonation offers high storage capacity (i.e. >
naturally occurring process in which Mg- or Ca-based min- 10,000 Gt of CO2), which means the worldwide supply of
erals react with CO2 to form environmentally friendly and minerals has the potential to sequester all future CO2 emis-
sions (Lackner et al. 1995). However, mineral sequestration
Responsible Editor: Philippe Garrigues for large-scale CO2 sequestration is not economically feasible
due to its high cost (Yadav and Mehra 2017a, b, 2019; Saran
* Anurag Mehra
et al. 2018; Cao et al. 2020). Therefore, mineral sequestration
[email protected]
is suggested for small- and medium-scale CO2 emitters, par-
Shashikant Yadav ticularly below 2.5 Mt of CO2. This accounts for about 10 to
[email protected]
15% of global CO2 emissions (Sanna et al. 2012b). The car-
1
Department of Chemical Engineering, Dr B R Ambedkar National
bonates are thermodynamically more stable than their primary
Institute of Technology Jalandhar (Punjab) India, minerals due to their lower energy state. Thus, the storage is
Jalandhar, Punjab 144011, India permanent and environmentally safe and there is little need for
2
Department of Chemical Engineering, Indian Institute of Technology monitoring (Saran et al. 2017; Yadav et al. 2017; Yadav and
Bombay, Powai, Mumbai 400076, India Mehra 2019). The carbon distribution in the Earth’s
Environ Sci Pollut Res (2021) 28:12202–12231 12203
Fig. 1 Different CO2 sequestration routes
lithosphere is the proof for the stability of mineral carbon- Mineral sequestration route
ation. About 50% of all carbon is present as limestone
(CaCO3) and other carbonates (Sanna et al. 2014). Most The mineral sequestration process can occur either below
mineral carbonation concerns relate to the use or disposal ground level (in situ) or above ground level (ex situ) (Jeon
of the carbonate produced during the process as the existing et al. 2018; Raza et al. 2018; Underschultz et al. 2018; Liu
market can only absorb a tiny portion of mineral carbon- et al. 2019a; Pastero et al. 2019; Wang et al. 2019). Below
ation products (Benhelal et al. 2018a, b; Ebrahimi et al. ground level, the process requires CO2 injection into un-
2018; Rahmani 2018; Leemann and Loser 2019). Other is- derground reservoirs which triggers a reaction between al-
sues that limit the effectiveness of mineral carbonation in kaline minerals and CO2 in geological formations. This
CO2 mitigation are slow kinetics of CO2, silicate reactions, reaction produces carbonates (Sipilä et al. 2008). Above
energy demands of pre-treatments, logistics and scalability ground level, processes involve rock mining and commi-
issues (Gerdemann et al. 2007; Sanna et al. 2012b, 2014; nution of the mineral ore as pre-processing for carbonation
Salek et al. 2013). (IPCC 2005; Sanna et al. 2014).
Table 1 Comparison of different CO2 sequestration routes
Storage types Benefits Drawbacks Potential, Gt
Geological Developed technology Threat of leakage 1800 (Shukla et al. 2010)

Economical Requires constant monitoring
Public acceptance Shortage of suitable sites
Ocean High potential High environmental risk > 1000 (Huijgen and Comans 2003)
Abundance Expensive than geological storage
No monitoring Negative/hostile perception
Biological Low cost Monoculture plantation can imbalance the ecosystem 100 (Paustian et al. 1998)
Less environmental issues Insufficient capacity
High potential Risk of disruption of food chain
Mineral carbonation Environmentally safe High costs > 10,000 to 10,000,000 (Teir 2008)
Exothermic reactions Energy intensive
Abundance of feedstock Slow reaction kinetics
Permanency Pre-treatment
Utilization of industrial wastes Unsecure future potential
Poor recovery of additives
Mining of feedstock creates environmental issues
Disposal or use of the process product if
implemented in large scale
12204 Environ Sci Pollut Res (2021) 28:12202–12231
Various methods have been reported in carbonation studies enhance the rate of reaction (Huijgen and Comans 2003).
for performing ex situ CO2 sequestration which are classified Steam conversion of any present oxides to hydroxide, a more
as direct carbonation and indirect carbonation (see Fig. 2). reactive substance capable of carbonation, also presents a so-
lution.
Direct carbonation
MgO ðsÞ þ H2 O ðgÞ→MgðOHÞ2 ðsÞ
Direct carbonation is the most straightforward method and MgðOHÞ2 ðsÞ þ CO2 ðg Þ→MgCO3 ðsÞ
consists of a single-process stage for carbonation (Liu et al.
2018b). Direct carbonation is further classified into two The process described above is performed by Kwon et al.
categories: gas–solid carbonation and direct aqueous (2011) in a dry environment, with the assumption of moisture
carbonation methods. Direct aqueous carbonation is within the flue gas as sufficient support for conversion of
generally used to compare other carbonation processes silicate oxides to comparatively more reactive hydroxides.
(Sanna et al. 2014). However, the process still requires large quantities of feed-
stock for CO2 sequestration due to low efficiency of carbon-
Direct gas–solid carbonation ation (Kwon et al. 2011).
The simplest carbonation method is the direct gas–solid car- Direct aqueous carbonation
bonation. This method was first successfully carried out by
Lackner et al. (1997). Several types of reactions are possible This approach employs ‘slurry’, which is an aqueous solution
by using different feedstock. The direct gas–solid carbonation composed of fine minerals. Dissolution of minerals and sub-
of olivine (Mg2SiO4) is provided as an example. sequent carbonation happen in a single reactor (Azdarpour
Mg2 SiO4 ðsÞ þ 2CO2 ðgÞ→2MgCO3 ðsÞ þ SiO2 ðsÞ et al. 2018; Li et al. 2018; Benhelal et al. 2019; Farhang
et al. 2019). This process is used for carbonation of Ca/Mg
Direct gas–solid carbonation showcases benefits such as silicates in an aqueous suspension (O’Connor et al. 2000;
simplicity in process design and possible recovery of heat at Gerdemann et al. 2007). Direct aqueous carbonation can be
high temperatures (Zevenhoven and Kavaliauskaite 2004). explained by three reaction stages:
However, due to slow reaction rate, this method is not viable
unless some optimizations are performed to accelerate the a. The leaching of minerals
carbonation process. Heat-activated feedstock is one way of
accelerating the carbonation, but it would require additional Mg2 SiO4 ðsÞ þ 4 Hþ ðaqÞ→2Mg2þ ðaqÞ þ 2H2 O ðlÞ
energy demands (Zevenhoven and Kohlmann 2001). CO2 in- þ SiO2 ðsÞ
jection at high pressure or using supercritical CO2 can also
Fig. 2 Different mineral CO2 sequestration routes

b. The dissolution of CO2 followed by release of carbonate solution plays a crucial role in reaction kinetics. High pH
ions functions as an effective CO2 vehicle and decreases reaction
time (O’Connor et al. 2005). The reaction between hydroxyl
CO2 ðgÞ þ H2 O ðlÞ→CO3 2– ðaqÞ þ 2Hþ ðaqÞ ion and gaseous CO2 causes almost instantaneous regenera-
tion of bicarbonate:
c. The nucleation and growth of mineral carbonates
OH− ðaqÞ þ CO2 ðgÞ→HCO−3 ðaqÞ
Mg2þ ðaqÞ þ CO3 2– ðaqÞ→MgCO3 ðsÞ
The solution maintains a constant HCO3− concentration
and pH, and there is no NaHCO3 consumption within the
This 3-step process occurs concurrently within a single
process.
reactor. CO2 dissolution takes place in water creating carbonic
Some salt additives form complexes from dissolved Mg
acid (H2CO3) which release hydrogen ions (H+) and bicarbon-
and Ca which reduce the activity of Mg and Ca in the solution
ate ions (HCO3−). The H+ causes hydrolysis of the mineral
causing an increased release of Mg and Ca ions from the
which releases the magnesium ions (Mg2+) and silica (SiO2).
silicate minerals (Olajire 2013). The release of Mg2+ ions from
Later, the Mg2+ and HCO3− ions react to form solid carbonate.
the silicate is increased by the addition of NaCl (Fauth et al.
Mineral dissolution is the slowest reaction step, but the
2000)
kinetics can be improved by silicate dissolution through addi-
tives and by altering conditions (Li and Hitch 2018; Wang Mg2þ ðaqÞ þ 2Cl– ðaqÞ→MgCl4 2– ; MgCl3 – ; MgCl2 ðaqÞ
et al. 2019). Altering conditions can be done through changes
to temperature, solid-to-liquid ratio, CO2 concentration, pres- Direct routes generally use a simple design. However, they
sure and particle size. Additive chemicals such as acids, bases require high CO2 pressure and temperature, and reaction rates
or salts can also be used to accelerate the reaction process. and conversions are low. Multiple physical and chemical pre-
Acids and complexing agents such as HCl, CH3COOH and treatments and mechanical and heat activation methods can
formic acid (HCOOH) serve as reaction accelerants (Lackner enhance mineral reactivity (McKelvy et al. 2004; Park and
2002; Huijgen 2007; Park et al. 2003). It is also observed that Fan 2004; Maroto-Valer et al. 2005; Teir 2008). Pre-
the combination of oxalic acid, orthophosphoric acid and eth- treatments can improve reaction rates and efficiency by in-
ylenediaminetetraacetic acid (EDTA) caused a significant increasing surface area (Li and Hitch 2018; Rashid et al. 2019;
crease in Mg2SiO4 dissolution (Park et al. 2003). Further im- Yu et al. 2019). However, chemical pre-treatments, along with
provements can be made to the chemistry of the solution other elements, reduce MgO content lowering mineral carbon-
through the addition of alkali metal hydroxides which enhance ation potential. Direct methods also suffer from large energy
the absorption of CO2 by increasing pH within the solution. requirements, which indirectly create more CO2 emissions
There is also no consumption of the hydroxide. Both HCO3− than what the process actually sequesters (O’Connor et al.
and OH− perform as catalysts. There is an optimal pH, which 2005; Teir 2008).
is dependent upon the preferred option for reaction with mag-
nesium: carbonate or bicarbonate ions. Another means of en- Indirect carbonation
hancing both dissolution of Mg2SiO4 and raising of pH is by
adding Na2CO3 (Huijgen and Comans 2003). Salt additives Indirect mineral carbonation process utilizes multiple stages
(e.g. NaCl, sodium bicarbonate (NaHCO3) and (Na/K)NO3) (Larisa et al. 2018; Martín et al. 2018b; Wang et al. 2018;
also accelerate the reaction by increasing ionic strength of the Zhao et al. 2019). Firstly, the ions of Mg or Ca are extracted
solution which reduces Ca/Mg activity within the solution that from the mineral ore through the use of acids or other solvents
favour the release of Mg2+/Ca2+ ions from the minerals and then converted to their respective oxides or hydroxides.
(O’Connor et al. 2000, 2005; Huijgen 2007). Subsequently, these oxides or hydroxides are allowed to react
with CO2 to form carbonates (Sipilä et al. 2008). Pure carbon-
NaHCO3 ðsÞ→Naþ ðaqÞ þ HCO−3 ðaqÞ ates can be produced from indirect methods given the impurity
Mg2 SiO4 ðsÞ þ 4Naþ ðaqÞ þ 4HCO−3 ðaqÞ→2MgCO3 ðsÞ extraction prior to carbonate precipitation stage (Bobicki et al.
2012; Eloneva et al. 2012). Most indirect processes typically
þ SiO2 ðsÞ þ 2Na2 CO3 ðaqÞ þ 2H2 O ðlÞ deliver faster carbonation than direct methods. There are sev-
Na2 CO3 ðaqÞ þ Hþ ðaqÞ þ HCO−3 ðaqÞ→2NaHCO3 ðaqÞ eral methods of indirect carbonation. They are as follows:
The NaHCO3 increases the concentration of HCO3−, there- Indirect gas–solid carbonation
by increasing the rate of reaction (Fauth et al. 2000). NaHCO3
addition makes solution slightly alkaline which raises solution Carbonation of Mg or Ca oxides or hydroxides is much faster
pH from 7.7 to 8.0 (O’Connor et al. 2001a). The pH of the than direct carbonation from their respective silicate forms.
But, Ca/Mg oxides/hydroxides rarely appear naturally. So, The main disadvantages of this method include excessive
producing them from Ca/Mg silicates is necessary. energy demands and high extraction costs for HCl recovery,
Hence, indirect gas–solid carbonation uses a multistage high setup costs on corrosion-resistant material and large wa-
process. Firstly, the extracted Ca or Mg is converted into ter requirements. Also, the presence of soluble chloride in
their respective oxides or hydroxides. Subsequently, these proximity to alkali metals results in the formation of alkali
mineral oxides or hydroxides undergo carbonation in dry metal chlorides. This makes HCl recovery difficult, causing
conditions (Teir 2008). Steam aids in producing more reactive unacceptable HCl loss. The preferred quantity of alkali metals
magnesium hydroxide (Mg(OH)2) or calcium hydroxide present in feedstock should be lesser than 1 wt%.
(Ca(OH)2). Unfortunately, solid wastes typically have a greater composi-
tion of alkali metals. Thus, the approach does not prove viable
CaSiO3 ðsÞ þ 2HCl→CaCl2 ðaqÞ þ H2 O ðaqÞ þ SiO2 ðsÞ
for sequestration from alkaline solid waste minerals (Huijgen
CaCl2 ðaqÞ þ 2H2 O ðaqÞ→CaðOHÞ2 ðsÞ þ 2HCl ðaqÞ and Comans 2003; Sipilä et al. 2008).
CaðOHÞ2 ðsÞ þ CO2 ðgÞ→CaCO3 ðsÞ þ H2 O ðlÞ Investigations also show dehydration and crystallization
consume four times more energy than the actual energy pro-
Lackner observed that it takes approximately 2 h for 100% duced by the power plant emitting CO2 (Newall et al. 2000;
Mg(OH)2 conversion to MgCO3 at 500 °C temperature and Huijgen 2007). Thus, the approach is not an energy efficient
340 bar pressure (Lackner et al. 1997). Butt observed that it method of carbon sequestration.
takes approximately 30 min for 90% conversion of Mg(OH)2
to MgCO3 for a particle size of 0.1 μm at 565 °C temperature Acetic acid Kakizawa et al. (2001) developed an improved
and 53 bar pressure (Butt et al. 1998). These high-carbonation indirect aqueous carbonation process, which accelerates
rate processes make it feasible for industrial applications. Ca2+ extraction from minerals with CH3COOH in the first
Hence, further studies on indirect gas–solid carbonation are step. It causes solid SiO2 precipitation and uses a thickener
recommended. to separate the SiO2. In the second step, CO2 is injected into
the solution, causing simultaneous carbonation of Ca and re-
covery of CH3COOH.
Indirect aqueous carbonation
CaSiO3 ðsÞ þ 2CH3 COOH ðlÞ→Ca2þ ðaqÞ þ SiO2 ðsÞ
Performing indirect aqueous carbonation involves a two-step þ 2CH3 COO– ðaqÞ þ H2 O ðlÞ
process consisting of extraction of Ca or Mg and, subsequent-
ly, its carbonation under aqueous conditions. The advantage Ca2þ ðaqÞ þ 2CH3 COO– ðaqÞ þ H2 O ðlÞ
of this route lies in the separate optimization of each step. The þ CO2 ðgÞ→CaCO3 ðsÞ↓ þ 2CH3 COOH ðlÞ
silicate rock dissolution is optimized with the use of different
acids and bases. The method also employs additive chemicals This method could provide 40% conversion at 25 °C tem-
to optimize carbonation (Ebrahimi et al. 2018; Liu et al. perature and 1 bar pressure. However, the conversion im-
2018a; Raza et al. 2018). Major indirect aqueous carbonation proved significantly to 75% when temperature and pressure
methods are explained below. were raised to 25 °C and 30 bar, respectively. The non-
corrosive quality of CH3COOH as compared to HCl makes
Hydrochloric acid This approach of indirect aqueous carbon- this approach a more viable method for carbonation.
ation utilizing hydrochloric acid involves converting calcium Employing the conventional method for precipitated calcium
silicates into carbonates in three stages (Lackner et al. 1995). carbonate (PCC) production using oil combustion for lime
The first step of the process extracts minerals, aided by HCl. calcination generates CO2 emissions to the order of 0.21 kg
Then, the solution is heated from 100 to 250 °C, a water- CO2 per kg of PCC produced. However, PCC production
vaporizing temperature, at which Ca(OH)2 precipitates and utilizing CH3COOH and wollastonite (CaSiO3) enables a
HCl is recovered simultaneously. Finally, the resulting 0.34 kg CO 2 sequestered per kg of PCC produced.
Ca(OH)2 is dissolved in water and allowed to react with However, large-scale deployment demands that the acid or
CO2 to form CaCO3. extraction agent is totally recycled and there is no evidence
to suggest that this can be done in an efficient and economical
CaSiO3 ðsÞ þ 2HCl ðlÞ→CaCl2 ðaqÞ þ H2 O ðaqÞ
manner (Peksa 2010). Also, large quantities of NaOH is re-
þ SiO2 ðsÞ quired to stimulate the carbonate precipitation from the acidic
solution, but this destroys the possibility of CH 3COOH
CaCl2 ðaqÞ þ 2H2 O ðlÞ→CaðOHÞ2 ðsÞ þ 2HCl ðlÞ
recycling further. Added to this, the reaction leaches out heavy
CaðOHÞ2 ðsÞ þ CO2 ðgÞ→CaCO3 ðsÞ þ H2 O ðlÞ metals causing impure carbonate precipitation. All these
factors effectively rule out this method for any kind of indus- 2NH4 Cl ðaqÞ þ CaðOHÞ2 ðaqÞ→2NH3 ðgÞ þ CaCl2 ðsÞ þ 2H2 O ðlÞ
trial application.
The general process can be defined
pH swing process The pH swing process is a two-step indirect 2NaCl ðsÞ þ 2CO2 ðgÞ þ CaðOHÞ2 ðsÞ→2NaHCO3 ðsÞ
aqueous carbonation process. In the first step, the pH of the
solution is reduced in order to boost the extraction of mineral þ CaCl2 ðsÞ
ions. In the second step, the pH of the solution is raised to
Finally, it is also possible to convert the bicarbonate to a
increase the carbonate precipitation (Larisa et al. 2018).
carbonate.
The pH swing process employs ammonium salts to im-
prove mineral dissolution efficiency, additive recovery and 2NaHCO3 ðsÞ→Na2 CO3 ðsÞ þ CO2 ðgÞ þ H2 O ðgÞ
reuse (Wang and Maroto-Valer 2011a, b, c). It forces gaseous
CO2 to interact with calcium chloride (CaCl2) and ammonia The Solvay process is not viable for industrial applications
(NH 3 ) in order to produce an ammonium carbonate given its large energy consumption and problems in recycling
((NH4)2CO3) and CaCl2 solution. This solution then goes to of NH3 because 1 mol of CO2 is formed for every 2 mol of
a precipitator for CaCO3 precipitation at a low pH, and am- CO2 sequestered by employing Ca(OH)2 to recycle NH3
monium chloride (NH4Cl) is recovered in this stage. The re- (Peksa 2010). A modified process that uses
covered NH4Cl then reacts with CaSiO3 in a separate vessel HOCH2CH2(CH3)NH instead of NH3 has been found to be
with raised pH to reform NH3 and CaCl2 for reuse. more energy efficient (Huang et al. 2001).
4NH4 Cl ðaqÞ þ 2CaSiO3 ðsÞ→2CaCl2 ðsÞ þ 4NH3 ðgÞ þ 2H2 O ðlÞ Precipitated calcium carbonate In studies pertaining to pro-
4NH3 ðgÞ þ 2CO2 ðgÞ þ 2H2 O ðlÞ duction of high-value PCC material with calcium silicates,
cost-effective calcium silicate sources were explored to re-
þ 2CaCl2 ðsÞ→2CaCO3 ðsÞ þ 4NH4 Cl ðaqÞ place the expensive wollastonite (Teir et al. 2007a). PCC is
primarily consumed by the paper industry with a high market
NH4Cl, (NH4)2SO4, NH4HSO4 and NH4HCO3 were inves- value (> $100/tonne) as it serves as a coating pigment and
tigated for the purpose of finding a suitable ammonium salt for paper filler that improves the quality of paper. Through pro-
the extraction of magnesium from Mg2SiO4 (Wang and cess modelling, it was revealed that CH3COOH was capable
Maroto-Valer 2011c). But, the experiments caused heavy of binding 0.34 tonne of CO2 per tonne of CaCO3 produced
NH3 loss. The application of NH4HCO3 proved more effec- whereas the earlier PCC production processes (with lime cal-
tive in the precipitation of hydromagnesite than the use of CO2 cination) emitted 0.21 tonne of CO2 per tonne of CaCO3
directly having the highest magnesium carbonation of 96%. It produced.
was determined that NH4HCO3 is the best absorbent with
extraction performance superior to even sulfuric acid, which Brine Oil and natural gas extraction processes produce brine as
was earlier believed to be the best. It was discovered that a waste product. There are huge quantities of brine stored in
magnesium extraction from Mg2SiO4 was also directly pro- surface storage tanks. Sufficient availability and a relatively
portional to temperature increases. With a particle size of 75 to high concentration of carbonate-forming metals (mainly Ca
150 μm, the dissolution rate of Mg2SiO4 was tested at several and Mg) make brine sequestration a viable carbonation meth-
temperatures. It was found by Wang and Maroto-Valer od (Doughty 2001; Kaszuba et al. 2005; Newton and Manning
(2011b) that, at a temperature of 100 °C and after a period 2006; Soong et al. 2006; Jeon et al. 2018). Despite the capa-
of 3 h, NH4HSO4 was able to provide 100% magnesium ex- bilities of brine, slow reaction kinetics limits the industrial
traction from minerals. However, this process is quite potent viability of the process. Changes to parameters such as the
for pure carbonate product but not suitable for industrial ap- composition of brine, its pH, temperature and/or pressure have
plications as it incurs high costs. an influence on the process kinetics (Ghomian et al. 2008;
Andreani et al. 2009; Xu et al. 2010; Kim et al. 2011;
Dual alkali approach This method is rooted in the Solvay Nyambura et al. 2011; Lu et al. 2012). But, how and how
process which employs NH3 as a catalyst in order to produce much still needs further research. Also, the availability of suit-
NaHCO3 and NaCl (Huang et al. 2001). The reaction has two able brine (with sufficient Ca and Mg composition) is limited,
phases: the saturation of brine with CO2 and NH3 and the use which makes this method less viable than approaches that
of lime with NH4Cl to recover NH3. utilize ultramafic rocks. Furthermore, when this method is
CO2 ðgÞ þ NaCl ðsÞ þ NH3 ðgÞ þ H2 O ðlÞ→NH4 Cl ðaqÞ used on a large scale, massive quantities of HCl are produced,
making waste disposal difficult (Kaszuba et al. 2003;
þ NaHCO3 ðsÞ Druckenmiller and Maroto-Valer 2005; Kharaka et al. 2009;
Ellis et al. 2010; Lopez et al. 2011; Liu et al. 2012).
Molten salt Use of molten salt (MgCl2·nH2O) rather than HCl of leaching a significant quantity of magnesium from
was found to increase energy efficiency by reducing dehydra- Mg2SiO4. Krevor and Lackner (2009) determined sodium cit-
tion energy requirements as the molten salt used was recycled rate salts, oxalates and EDTA improve the dissolution of
during the process (Huijgen 2007). Hence, molten salt was Mg2SiO4 in mildly acidic conditions substantially. The main
found to be a viable carbonation method (IEA-GHG 2000). challenge of chemically enhanced methods typically consists
There are two ways for carbonation using molten salt se- of additive recovery. However, they offer improvement on
questration method: pure material production which is valuable for other
applications.
i) The production and carbonation of Mg(OH)2 are per- High costs, use of makeup chemicals and high energy con-
formed and MgCl2·3.5H2O is utilized as a solvent for sumption make processes employing corrosive chemicals,
the production of Mg(OH)2. specifically HCl and MgCl2, economically unappealing.
Furthermore, chemical use without recycling must be avoided,
The Mg3Si2O5(OH)4 is first dissolved within the molten considering its costs and the potential environmental impact of
salt at a temperature of 200 °C: large-scale industrial sequestration (Olajire 2013).
Indirect aqueous mineral carbonation, though feasible in
Mg3 Si2 O5 ðOHÞ4 ðsÞ þ 3MgCl2 terms of technology and energy, has high costs. Possible
3:5H2 Oð1Þ→6MgðOHÞClðlÞ þ 2SiO2 ðaqÞ þ 9:5H2 Oð1Þ routes to cost reduction in ex situ indirect aqueous mineral
carbonation are large-scale reactor development, sophisticated
The silica is separated at T = 150 °C and water is added additive development and development of an integrated CCS
which causes the precipitation of Mg(OH)2. process.
2MgðOHÞClðlÞ þ nH2 OðlÞ→MgCl2 nH2 OðlÞ
þ MgðOHÞ2 ðsÞ
Suitable feedstock
Mg(OH)2 is separated and then carbonated
Both the natural minerals and industrial waste and by-
MgðOHÞ2 ðsÞ þ CO2 ðgÞ→MgCO3 ðsÞ þ H2 OðgÞ products rich in Mg and Ca can be used as a CO2 sequestration
feedstock. A brief description of both types of materials is
given in the following:
ii) Direct carbonation of MgCl2·3.5H2O (l).
Natural minerals
MgCl2 3:5H2 Oð1Þ
Mg3 Si2 O5 ðOHÞ4 ðsÞ þ 3CO2 ðgÞ → 3MgCO3 ðsÞ
Mg- and Ca-based minerals such as wollastonite (CaSiO3)
þ 2SiO2 ðsÞ þ 2H2 OðlÞ and forsterite (Mg2SiO4) have been deemed the most suit-
able for carbonation as a part of the CO2 sequestration
The CO2 pressure is roughly maintained at 30 bar (Newall process (see Table 3). Apart from alkaline earth minerals,
et al. 2000). A significant disadvantage of this method is the other elements such as alkali metals (K and Na) and many
corrosive nature of the solvent used which causes construc- other metals (e.g. Fe, Al, Zn, Cu, Mn, Ni and Co) are also
tional as well as operational problems. Moreover, despite used in CO2 sequestration. But, alkali metals are less pre-
recycling of the molten salt, additives such as MgCl 2· ferred because their final products are soluble in water,
3.5H2O are needed. It was concluded that sufficient supply which, in turn, weaken the CO2 sequestration process.
of MgCl2 was not recycled in the process to make this method Pan et al. (2012) and Teir (2008) reported the problems
viable for industrial applications (Newall et al. 2000). Hence, associated with the use of alkali metal–based feedstock
this method has been rejected as a suitable carbonation meth- for long-term CO2 sequestration. Similarly, metals such
od (Sipilä et al. 2008). as Fe, Al, Mn, Cu, Co, Zn and Ni are not economically
viable to be abundantly used as a raw material for CO2
Use of other chemical additives in mineral carbonation sequestration (Teir 2008). It was found that a sufficient
Investigations of silicate rock dissolution explored a wide set amount of iron is available on Earth which can be utilized
of other acids and bases than the ones discussed above (see as feedstock for CO2 sequestration, but utilization of the
Table 2) such as H2SO4, NaOH, CH3COONH4, NH4NO3 and valuable metal is unadvisable (Huijgen and Comans 2003).
NH4HSO4 (Doucet 2010; Eloneva et al. 2012; Dri et al. 2013). Natural minerals suitable for CO2 sequestration are broadly
Teir et al. (2007c) found CH3COOH and HCOOH are capable classified into two categories.
Table 2 List of chemicals used

for mineral carbonation Solvent References
Acetic acid (Kakizawa et al. 2001; Huijgen and Comans 2003; Teir et al. 2007a, c; Eloneva
et al. 2008a, b; Fagerlund et al. 2009; Bałdyga et al. 2010; Bao et al. 2010;
Bobicki et al. 2012)
Ammonium chloride (Kodama et al. 2008; Krevor and Lackner 2009; Eloneva et al. 2012; Said et al.
2013)
Ammonium sulfate (Fagerlund et al. 2009, 2012; Power et al. 2010; Wang and Maroto-Valer 2011a,
b, c; Highfield et al. 2012; Nduagu et al. 2012)
Citric acid (Prigiobbe et al. 2009b, c)
Hydrochloric acid (Lackner et al. 1995; Teir et al. 2007b, c, 2009; Lin et al. 2008; Fagerlund et al.
2009; Li et al. 2009; Prigiobbe et al. 2009b, c; Haug et al. 2010; Zhao et al.
2010)
Lithium hydroxide (Prigiobbe et al. 2009a, b, c)
Nitric acid (Teir et al. 2007b, c, 2009; Fagerlund et al. 2009; Doucet 2010)
Sodium bicarbonate (Gerdemann et al. 2007; Andreani et al. 2009; Jarvis et al. 2009; Koukouzas
et al. 2009; Verduyna et al. 2011; Sanna et al. 2013b)
Sodium chloride (Gerdemann et al. 2007; Andreani et al. 2009; Dufaud et al. 2009; Koukouzas
et al. 2009; Krevor and Lackner 2009; Li et al. 2009; Prigiobbe et al. 2009a, b,
c; Mayoral et al. 2013)
Sodium hydroxide (Maroto-Valer et al. 2005; Alexander et al. 2007; Teir et al. 2007b, 2009;
Eloneva et al. 2008a, b; Lin et al. 2008; Daval et al. 2009a, c; Fagerlund et al.
2009; Li et al. 2009; Doucet 2010)
Sodium nitrate (Prigiobbe et al. 2009a, b, c)
Sulfuric acid (Maroto-Valer et al. 2005; Alexander et al. 2007; Teir et al. 2007c; Fagerlund
et al. 2009; Doucet 2010)
Natural magnesium silicates in soil amendment (Maroto-Valer et al. 2005). Theoretically,

1 tonne of olivine can sequester 2/3 tonnes of CO2.
Magnesium silicates are the most abundant mineral feed-
Mg2 SiO4 ðsÞ þ 2CO2 ðgÞ→2MgCO3 ðsÞ þ SiO2 ðsÞ
stock for CO2 mineralization. Olivine (Mg2SiO4) and ser-
pentine (Mg3Si2O5(OH)4) have been the predominant sil-
icates in mineral carbonation research because of the na- The exothermic reaction of olivine carbonation has a −
ture of magnesium silicate rocks, which are typically 95 kJ/mol enthalpy of reaction. Direct aqueous carbonation
richer in base ions compared to calcium silicate rocks at 25 to 90 °C and ambient pressure is the most studied car-
(Li and Hitch 2018; Li et al. 2018, 2019; Wang et al. bonation route. Carbonation process, however, is slow under
2019). In rocks, magnesium silicates exist in various ambient conditions. So, reaction parameters are optimized to
forms such as serpentinites, peridotites and dunites. enhance the reaction rate to make the carbonation process
Dunite primarily consists of olivine while peridotite is industrially attractive (Seifritz 1990; Kwon et al. 2011).
predominantly olivine and pyroxene. Serpentinite consists Maximum conversion was observed at temperatures of 150–
of mainly magnesium silicates in the form of serpentine. 200 °C and pressures close to 250 bar (O’Connor et al. 2005).
Since magnesium silicates are available on such a large Rate of carbonation reaction can be increased by the use of
scale, their theoretical storage capacity is estimated to be inorganic salts as additives such as NaHCO3, KHCO3 and
large enough to host all the CO2 released from the oxida- NaCl (Giammar et al. 2005; O’Connor et al. 2005).
tion of all the fossil fuel reservoirs present on Earth O’Connor et al. (2001b) conducted experiments at 185 °C
(Huijgen and Comans 2003). temperature and 115 bar pressure with 37 μm particle size
and achieved 91% conversion in 24 h. Another experiment
Olivine Olivine is a leading mineral feedstock for CO2 seques- which used a different salt concentration of 0.5 M NaOH +
tration process due to its high reactivity, cheap availability 1 M NaCl achieved 84% carbonation within 6 h. Pre-treatment
($4–5/tonne) due to its abundance and high storage capability of feedstock such as magnetic separation, mechanical activa-
(Lackner et al. 1995; Maroto-Valer et al. 2005; Kwon et al. tion, chemical activation and heat activation was found to
2011). Additionally, the carbonation product has applications increase the reaction rate (Maroto-Valer et al. 2005; Baláž
Table 3 List of potential minerals investigated for mineral carbonation
Minerals Chemical formula References
Basalt Based on rock formation (O’Connor et al. 2005; Teir et al. 2005; Assayag et al. 2009; Matter et al. 2009;
Schaef et al. 2009; Gislason et al. 2010; Goldberg et al. 2010)
Brines (Druckenmiller and Maroto-Valer 2005; Soong et al. 2006; Nyambura et al. 2011)
Brucite Mg(OH)2 (Lackner et al. 1997; Chen et al. 2006; Hänchen et al. 2008; Zevenhoven et al. 2008;
Zhao et al. 2010)
Chrysotile Mg3(Si2O5)(OH)4 (Dufaud et al. 2009)
Dunite 90% Olivine (Andreani et al. 2009; Koukouzas et al. 2009)
Feldspar CaAl2Si2O8 (O’Connor et al. 2005)
Forsterite Mg2SiO4 (Golubev et al. 2005; Bali et al. 2008; Kwak et al. 2010)
Harzburgite CaMgSi2O6 + (Fe, Al) (Koukouzas et al. 2009)
Listwanite Carbonated serpentinite (Hansen et al. 2005)
Olivine (Mg, Fe)2SiO4 (Maroto-Valer et al. 2005; O’Connor et al. 2005; Penner et al. 2005; Beärat et al.
2006; Chen et al. 2006; Schuiling and Krijgsman 2006; Hanchen et al. 2006;
Khoo and Tan 2006; Kleiv and Thornhill 2006; Gerdemann et al. 2007; Hänchen
et al. 2007; Baláž et al. 2008; Munz et al. 2009; Prigiobbe et al. 2009a, b, c;
Dufaud et al. 2009; Kwak et al. 2010, 2011; Fabian et al. 2010; Kwon et al. 2011;
Verduyna et al. 2011)
Peridotite Based on rock formation (Kelemen and Matter 2008; Matter and Kelemen 2009; Rudge et al. 2010)
Pyroxene CaMgSi2O6 + (Fe, Al) (O’Connor et al. 2005; Dufaud et al. 2009)
Pyroxenite Pyroxene rocks (Koukouzas et al. 2009)
Serpentine Mg3Si2O5(OH)4 (Lackner et al. 1997; Park et al. 2003; Park and Fan 2004; O’Connor et al. 2005;
Hršak et al. 2005; Chen et al. 2006; Cheng and Hsu 2006; Khoo and Tan 2006;
Alexander et al. 2007; Gerdemann et al. 2007; Lin et al. 2008; Zevenhoven et al.
2008; Li et al. 2009; Krevor and Lackner 2009, 2011; Verduyna et al. 2011; Wang
and Maroto-Valer 2011a, c; Nduagu et al. 2012; Fagerlund et al. 2012; Highfield
et al. 2012; Wee 2013)
Serpentinite Based on rock formation (Teir et al. 2007b, c, 2009; Boschi et al. 2009; Fagerlund et al. 2009)
Slaked lime Ca(OH)2 (Domingo et al. 2006; Feng et al. 2007)
Talc Mg3Si4O10(OH)2 (O’Connor et al. 2005)
Wollastonite CaSiO3 (Kakizawa et al. 2001; Teir et al. 2005, 2007a; O’Connor et al. 2005; Huijgen et al.
2006a, b, 2007; Khoo and Tan 2006; Gerdemann et al. 2007; Daval et al. 2009b,
c; Bałdyga et al. 2010)
et al. 2008). However, the high cost of pre-treatment substan- of serpentine-rich tailings already piled up due to mining of
tially increases the overall cost of the carbonation process serpentine-rich ultramafic rocks for several industrial applica-
(Maroto-Valer et al. 2005; Kwon et al. 2011). Summers tions can also be utilized for mineral carbonation which helps
et al. (2005) studied the effect of mechanical activation on avoid mining costs as well as reduce hazardous characteristics
olivine carbonation at 185 °C temperature and 150 bar pres- of serpentine tailings. The total amount of serpentine at chro-
sure for a period of 1 h by using different grinding methods. mium, nickel and talc mines in Finland is around 29 Mt (Teir
This experiment yielded a 5.1% conversion with the use of et al. 2009). However, serpentine carbonation has a low car-
inactivated olivine. However, the conversion increased to bonation rate. Pre-treatment of serpentine feedstock and use of
69.9% through the use of stirred media detritor (SMD) mill additives such as inorganic salts and acids have been investi-
wet grinding and the use of attrition mill (AM) wet grinding gated to increase the mineral dissolution, reaction rate and
for 1 h yielded a still higher conversion of 84.3% (Summers total carbonation (Teir et al. 2007b, c; Olajire 2013; Sanna
et al. 2005). et al. 2013b). One tonne of serpentine can theoretically se-
quester 1/2 tonnes of CO2.
Serpentine Though serpentine is less reactive than olivine, its
wide availability in large amounts makes it suitable as an Mg3 Si2 O5 ðOHÞ4 ðsÞ þ 3CO2 ðgÞ→3MgCO3 ðsÞ
economical feedstock for mineral carbonation (Jonckbloedt þ 2SiO2 ðsÞ þ 2H2 O ðlÞ
1998; O’Connor et al. 2005). Additionally, large quantities
This reaction is exothermic, and enthalpy of the reaction is 2018; Liu et al. 2018b, 2019b; Wang et al. 2018; Huang et al.
− 64 kJ/mol. Lackner et al. (1997) used direct aqueous car- 2019; Leemann and Loser 2019).
bonation method with a temperature range of 140 to 300 °C Various waste materials have been considered for carbon-
and pressure of 340 bar to achieve 30% conversion after ation (Huijgen et al. 2005b; Teir et al. 2007a; Kodama et al.
240 h. Similarly, O’Connor et al. (2001b) achieved 34% car- 2008; Lekakh et al. 2008; Teir 2008). Waste materials such as
bonation after 24 h of reaction at 185 °C temperature and a cement dust (Huntzinger 2009), coal fly ashes (Back et al.
pressure of 115 bar. O’Connor et al. (2001b) also found that 2008; Uibu 2008) and concrete waste (Iizuka et al. 2004;
the total carbonation increased to 83% within 6 h of reaction Shtepenko et al. 2005; Stolaroff et al. 2005) have been tested
by using heat-activated serpentine and a salt solution (1 M for mineral carbonation. However, waste residue with high
NaCl + 0.5 M NaHCO3). Several acids and bases were also quantities of alkaline earth metals, such as Ca and Mg, is often
used to increase the dissolution of serpentine and, subsequent- preferred (see Table 4). For any tested material to be selected
ly, the carbonation reaction rate (Maroto-Valer et al. 2005; for carbonation, it should have desirable quantities of Mg or
Teir et al. 2007c; Sanna et al. 2014). Teir et al. (2007c) con- Ca readily available in the desired mineral phase.
ducted leaching experiments using several solvents to identify Certain mineral wastes such as air pollution control (APC)
the most appropriate solvent. It was observed that the efficien- waste (Baciocchi et al. 2006, 2009a; Li et al. 2007), steel slag
cy of Mg extraction from serpentinite was highest for H2SO4, (Huijgen et al. 2005b), oil shale ash (Reddy et al. 1991) and
followed by HCl, HNO3, HCOOH and then CH3COOH (Teir bottom ash (Van Gerven et al. 2005) have been found suitable
et al. 2007c). However, pre-treatment of serpentine and usage for mineral carbonation. Also, the use of these mineral wastes
of any additive chemical substantially increase the cost of the for carbonation makes them more stable by reducing their
process just as in the case of olivine carbonation (O’Connor leaching activity and thus enabling their use in industrial ap-
et al. 2005; Sanna et al. 2012a). plications or meeting landfill acceptance criteria (Abid et al.
2018; Zhu et al. 2018; Chang et al. 2019).
Natural calcium silicates
Steelmaking slags
Wollastonite Among calcium silicate minerals, wollastonite
Steel manufacturing industries are one of the highest CO2
(CaSiO3) is believed to be the most suitable naturally occur-
emitters in the world. They contribute roughly 6 to 7% of
ring mineral for CO2 sequestration. Wollastonite has a high
the overall CO2 produced (Doucet 2010). For every single
Ca content with theoretical composition is 51.7% SiO2 and
tonne of iron steel manufactured, 0.28–1.0 tonne of CO2 is
48.3% CaO, which has a huge potential to produce stable
released into the atmosphere (Bonenfant et al. 2008c). About
carbonates (Huang et al. 2019; Xu et al. 2019). Wollastonite
10–15% of the steel production process output is in the form
has a faster reaction rate compared to Mg silicate and also
of residues known as slags. These slags, however, can con-
lacks substantial industrial applications (O’Connor et al.
tribute significantly as feedstock for mineral carbonation
2005). Unfortunately, global availability of wollastonite is
(Proctor et al. 2000; Gerdemann et al. 2007). It is estimated
low and some studies conclude that it is not viable due to its
that, roughly, 218–262 Mt and 124–186 Mt of iron and steel
scarcity (Lackner 2002). However, in places like India, which
slag, respectively, were produced in the year 2006 alone (van
is the second largest wollastonite producer in the world (pro-
Oss 2007). It is also found that steelmaking slags can hold up
duction was 141,550 tonnes in 2012–2013), inadequacies are
to 171 Mt of CO2 per year globally which amounts to storing
not an issue and wollastonite presents a more valuable pro-
0.6% of global CO2 emissions annually (Eloneva et al.
posal for CO2 sequestration (IBM 2015).
2008a).
Four types of slags are obtained during steel production,
Industrial wastes namely electric arc furnace (EAF) slag, blast furnace (BF)
slag, ladle furnace (LF) slag and basic oxygen furnace
Natural minerals are sourced through mining, and the process (BOF) slag (Teir et al. 2007a; Eloneva et al. 2010). These
is energy intensive and also has adverse environmental im- slags constitute mostly of oxides and silicates of metals, such
pacts. However, waste residues are cheap and readily avail- as Fe, Al, Ca, Mn and Mg. There are also traces of other
able and their carbonation has little negative impact on the elements such as Ti, Ni and Cr present in different phases
environment. However, their availability is limited compared (Motz and Geiseler 2001; Bonenfant et al. 2008c). The com-
to natural silicate minerals. But, waste residues can be effec- position of slags varies significantly even across batches com-
tive in facilities producing both CO2 and alkaline waste resi- ing from the same plant which is attributed to the type of steel
dues where availability will not be a concern. Therefore, using produced, the type of raw materials used and other factors (Shi
waste residues instead of natural minerals such as wollastonite 2004; Teir et al. 2007a). Generally, steel slags with high alka-
and olivine is recommended in such applications (Faisal et al. line content (pH ~ 12) and high Ca levels (32–52% CaO) are
Table 4 List of potential industrial and municipal wastes investigated for mineral carbonation
Waste materials Classification References
Biomass ash (Gunning et al. 2010)

Cement wastes CKD (Gunning et al. 2009, 2010; Huntzinger 2009; Sanna et al. 2012a)
CBD (Gunning et al. 2009, 2010)
Waste cement (Iizuka et al. 2004; Katsuyama et al. 2005; Stolaroff et al. 2005;
Kashef-Haghighi and Ghoshal 2010; Teramura et al. 2012)
Fuel combustion ashes Coal FA (Schramke 1992; Reddy et al. 1994; Tawfic et al. 1995; Montes-Hernandez et al.
2009; Nyambura et al. 2011; Sanna et al. 2012a; Muriithi et al. 2013)
Lignite FA (Soong et al. 2006; Back et al. 2008; Mayoral et al. 2013)
OS FA PF, CFB (Kuusik et al. 2005; Uibu et al. 2009, 2011)
WA (Gunning et al. 2010)
Iron and steel slags BFS (Monkman and Shao 2006; Eloneva et al. 2008b)(Monkman and Shao 2006;
Teir et al. 2007a; Eloneva et al. 2008b; Pan et al. 2012; Sanna et al. 2012a)
BOFS (Shi 2004; Huijgen et al. 2005c; Teir et al. 2007a; Teir 2008; Eloneva et al.
2008a, 2010; Kodama et al. 2008; Bao et al. 2010; Doucet 2010; Chang et al.
2011a, 2012, 2013; Sanna et al. 2012a)
EAFS (Shi 2004; Monkman and Shao 2006; Teir et al. 2007a; Bonenfant et al. 2008c;
Baciocchi et al. 2009b; Doucet 2010; Uibu et al. 2011; Sanna et al. 2012a)
LFS (Shin et al. 2004; Back et al. 2008; Bonenfant et al. 2008c; Uliasz-Bocheńczyk
et al. 2009; Uibua et al. 2011)
AODS (Teir et al. 2007a; Teir 2008; Baciocchi et al. 2009b; Sanna et al. 2012a; Santos
et al. 2012, 2013, 2014)
Mine tailings (Wilson et al. 2006, 2009; Bonenfant et al. 2008a; Hitch et al. 2010; Larachi
et al. 2010; Power et al. 2010; Sahu et al. 2010; Yadav et al. 2010; Bobicki
et al. 2012)
MSWI ashes MSWI BA (Meima and Comans 1997; Fernández Bertos et al. 2004b; Polettini and Pomi
2004; Van Gerven et al. 2005; Arickx et al. 2006; Cornelis et al. 2006;
Todorovic and Ecke 2006; Dijkstra et al. 2006; Rendek et al. 2006, 2007;
Costa et al. 2007; Gunning et al. 2010; Sanna et al. 2012a)
APC residue (Ecke 2003; Ecke et al. 2003; Fernández Bertos et al. 2004b; Astrup et al. 2005,
2006a, b; Baciocchi et al. 2006, 2009a; Li et al. 2007; Sun et al. 2008;
Prigiobbe et al. 2009d; Sanna et al. 2012a)
Oil shale ashes (Essington et al. 1991; Reddy et al. 1991, 1994; Uibu et al. 2010)
Paper mill wastes (Pérez-López et al. 2008; Gunning et al. 2009, 2010)
Red mud (Bonenfant et al. 2008a; Johnston et al. 2010; Sahu et al. 2010; Yadav et al.
2010; Si et al. 2013)
considered favourable for mineral carbon sequestration Direct aqueous carbonation process demonstrated to be
(Eloneva et al. 2008a). successful from the studies of Huijgen et al. (2005b),
Though the comminution process to make steel slags Lekakh et al. (2008) and Bonenfant et al. (2008c). A reason-
suitable for carbonation is expensive, it is still more cost- able extent of carbonation was achieved at both ambient and
effective compared to the mining and transportation costs increased pressure and temperature conditions (Table 5). In
involved when natural minerals are used. The carbonation the former scenario, 24.7% carbonation was attained
process proves economically beneficial by converting steel (Bonenfant et al. 2008c) while, in the latter case, with
slag to high purity–precipitated CaCO3 (Teir et al. 2007a; 100 °C temperature and 19 bar pressure, 74% carbonation
Eloneva et al. 2008b; Kodama et al. 2008). Moreover, the was attained (Huijgen et al. 2005b). Residues with high Ca
carbonation process increases the mechanical properties of content are considered more reactive. In fact, slags containing
steel slags and makes it appropriate for industrial applica- large amounts of CaO or Ca(OH)2 are found to be more reac-
tions (Fernández Bertos et al. 2004a; Huijgen et al. 2005b; tive than the ones with calcium silicate (Bonenfant et al.
Baciocchi et al. 2006, 2009b; Costa 2006; Rendek et al. 2008c). The process of carbonation is considerably quick
2006; Li et al. 2007). when temperature and pressure are increased (Huijgen et al.
Table 5 A summary of carbonation experiments performed under different reaction conditions
Materials Temperature Pressure Particle size L/S Solution Time CO2 uptake Conversion References
(°C) (bar) (μm) (h) (g/kg) (%)
BF slag 25 3 0.125 mL/g Wet carbonation 24 3 9 (Johnson 2000)

Stainless steel slag 25 3 0.125 mL/g Wet carbonation 24 210 21 (Johnson 2000)
Steelmaking slags 30 1 125–250 5 mL/g Indirect aqueous carbonation using 2 90 22.5 (Eloneva et al. 2008a)
0.1 M acetic acid and 46 g (NaOH)/L
BOF slag 70 1 < 44 10 mL/g Aqueous carbonation using DI water 2 229 57 (Chang et al. 2011a)
BOF slag 60 l.5 ~ 62 20 mL/g Aqueous carbonation using DI water 0.5 289 93.5 (Chang et al. 2012)
LD slag 100 19 < 38 10 g/g Aqueous carbonation using DI water 0.5 250 74 (Huijgen et al. 2005b)
BF slag 30 1 125–250 pH swing using CH3COOH and NaOH 2 227 90 (Eloneva et al. 2008b)
Environ Sci Pollut Res (2021) 28:12202–12231
(40 g/L)
Converter slag 40 1 < 63 Indirect aqueous carbonation using 1 80 (Kodama et al. 2008)
NH4Cl
EAF and AOD slag 50 3 0.4 mL/g Aqueous carbonation 2 130 (Baciocchi et al. 2009b)
LF slag Ambient 1 38–106 10 g/g Direct aqueous carbonation 40 247 47.5 (Bonenfant et al. 2008b)
EAF slag Ambient 1 45–75 4/3 mg/mL Direct aqueous carbonation 40 38 11 (Lekakh et al. 2008)
Cement-immobilised 50 250 80–1000 Direct carbonation of a mixture of slag, 0.25 14.8 (Van Ginneken et al. 2004)
slag sand, Portland cement, sand,
porphyry and water using
supercritical CO2
OPC cement 25 3 0.125 mL/g Wet carbonation 24 22 22 (Johnson 2000)
Portland cement 59 97 0.6 g/g Direct carbonation of cement paste 24 162 (Short et al. 2001)
Portland cement Ambient 2 < 250 Wet Direct carbonation of cement paste with 72 99 26 (Gunning et al. 2010)
water
Waste cement Ambient 4 < 80 1 mL/g Direct carbonation 0.8 33 16.5 (Teramura et al. 2000)
Cement kiln dust Ambient 1 Direct gas carbonation, relative 81 203 75.0 (Huntzinger et al. 2009)
humidity of gas > 98%, gravimetric
water content of waste 75%
BHC 160 48 < 44 10 mL/g Aqueous carbonation using DI water 12 283 68 (Chang et al. 2011b)
BHC 160 90 < 44 10 mL/g Aqueous carbonation using DI water 1 245 59 (Chang et al. 2011b)
BHC 70 1 < 44 10 mL/g Aqueous carbonation using DI water 2 187 44 (Chang et al. 2011a)
Coal FA 25 2.8 < 0.25 20% moisture 120 80 (Reddy et al. 1994)
Coal FA 30 10 ~ 40 10 mL/g Direct aqueous carbonation 18 26 65 (Montes-Hernandez et al.
2009)
Coal FA Ambient 10 0.6 g/g Direct aqueous carbonation 24 78.5 56.07 (Uliasz-Bocheńczyk et al.
FA/water 2009)
Coal FA 20 13.6 Direct aqueous carbonation of brine 2 219 (Soong et al. 2006)
using pH adjustment by 10% FA and
NaOH
Coal FA 30 40 20–150 0.5 g/mL Aqueous carbonation using brine solution 1 71.8 86.4 (Nyambura et al. 2011)
12213
Table 5 (continued)
12214
Materials Temperature Pressure Particle size L/S Solution Time CO2 uptake Conversion References
(°C) (bar) (μm) (h) (g/kg) (%)
Coal FA 30 1 ~ 40 10 g/g Aqueous carbonation using DI water 18 26 82 (Montes-Hernandez et al.

2009)
FBC coal ash 155 75 0.5 M Na2CO3/0.5 M NaHCO3/1.0 M 1 159 51 (Fauth et al. 2002)
NaCl
FGD coal ash 185 115 0.5 M Na2CO3/0.5 M NaHCO3/1.0 M 1 191 72 (Fauth et al. 2002)
NaCl
MSWI ash 25 3 0.125 mL/g Wet carbonation 24 60–140 39–50 (Johnson 2000)
MSWI BA Ambient 17 < 4000 20% moisture Direct gas–solid carbonation 3.5 47.52 (Rendek et al. 2006)
g/g
MSWI BA Ambient 3 < 710 0.3–0.4 g/g Direct gas–solid carbonation with 65% 2.5 31.9 75 (Fernández Bertos et al.
relative humidity 2004b)
MSWI FA/APC 21 3 0.3 g/g Direct gas–solid carbonation with 75% 3 100 12 (Li et al. 2007)
relative humidity
MSWI FA/APC Ambient 3 < 212 0.2–0.3 g/g Direct gas–solid with 65% relative hu- 2.5 73.1 75 (Fernández Bertos et al.
midity 2004b)
MSWI FA Ambient 1 0.142–632.5 0.25 g/g Aqueous carbonation using DI water 240 120 (Wang et al. 2010)
APC residues 30 1 0.2 g/g Aqueous carbonation using DI water 5 250 65 (Baciocchi et al. 2009a)
MSWI APC 20 1 2.5 mL/g Aqueous carbonation using DI water 3 200 (Cappai et al. 2012)
Oil shale ash Ambient 1 ~ 28 10 Aqueous carbonation 168 17.1 21.18 (Uibu et al. 2009)
Oil shale ash Ambient 1 ~ 43 10 g/g Aqueous carbonation using DI water 120 149.9 (Uibu and Kuusik 2009)
Oil shale ash Ambient 1 Direct aqueous using continuous-flow 120 170–200 98 (Uibu et al. 2010)
reactor
Spent oil shale 25 2.8 < 0.25 0.2 g/g Direct gas-phase carbonation 120 80 (Reddy et al. 1994)
Deinking ash 25 3 0.125 mL/g Wet carbonation 24 170 17 (Johnson 2000)
Pulverised fuel ash 25 3 0.125 mL/g Wet carbonation 24 15 57 (Johnson 2000)
Paper mill waste 30 10 ~ 15 L/S = 50 Aqueous carbonation using DI water 2 218 85 (Pérez-López et al. 2008)
Red mud Ambient 3.5 ~ 30 0.35 mL/g Direct aqueous carbonation 3.5 53 21.86 (Yadav et al. 2010)
Red mud Ambient 1 < 160 10 mL/g Direct aqueous carbonation 72 263.3 (Sahu et al. 2010)
Red mud 20 1 < 1000 10 mL/g Direct aqueous carbonation 24 41.5 21.84 (Bonenfant et al. 2008a)
Red mud Ambient 1 5 mL/g Direct aqueous using brine and 0.5 17 (Johnston et al. 2010)
overnight settling
Asbestos tailings Ambient 1 Passive (tailings piles) 8760 0.3 (Wilson et al. 2009)
Asbestos tailings 375 1 37–75 80 mL/g Direct gas–solid carbonation 5 22 0.5 (Larachi et al. 2010)
Nickel tailings 30 1 0–500 Indirect aqueous carbonation using 4 M 0.67 404 94 (Teir et al. 2007b)
HCl or HNO3 and NaOH
Bauxite residue Ambient 1 Aqueous carbonation of 5 g slurry 720 21 (Khaitan et al. 2009)
Olivine 185 150 < 38 15% solid 0.64 M NaHCO3, 1 M NaCl 1 49.5 (Gerdemann et al. 2007)
Environ Sci Pollut Res (2021) 28:12202–12231
(Maroto-Valer et al. 2005)

2005b; Bonenfant et al. 2008c; Lekakh et al. 2008). Indirect
(Gerdemann et al. 2007)

aqueous carbonation which involves the separation of disso-
(Huijgen et al. 2006a)

(Bałdyga et al. 2010)
(Park and Fan 2004)
(Kwak et al. 2010)
lution and precipitation processes in slag carbonation has also
(Lin et al. 2008)

been found successful. Essentially, it is meant to enhance the
References
entire process through pH adjustment for dissolution and pre-

cipitation steps individually through the use of additives (Teir
et al. 2007a; Eloneva et al. 2008b, a; Kodama et al. 2008) and
altering pressure or temperature conditions (Iizuka et al.
Conversion
2004).
73.5
(%)
Cement wastes
75
90
26
65
60
8
Cement manufacturing industries release considerably high

CO2 uptake
quantities of CO2 into the atmosphere which is about 5% of

global CO 2 emissions (Huntzinger and Eatmon 2009;
(g/kg)
Huntzinger et al. 2009). The total annual production of cement

is estimated to be 2.8 Gt currently and expected to rise to 4 Gt
Time
0.25
(Schneider et al. 2011). Due to the availability of cement

(h)
20
26
1
1
wastes in abundance, ease of carbonation and potential for

0.6 M NaHCO3; 1.0 M NaCl solution in
Indirect carbonation using succinic acid

1 vol% orthophosphoric acid, 0.9 wt%
waste recycling, cement wastes presents a very suitable source

of oxalic acid and 0.1 wt% EDTA
for mineral carbonation (Huijgen and Comans 2003;

Indirect carbonation using 1 N
Fernández Bertos et al. 2004c; IPCC 2005; Shtepenko et al.

0.64 M NaHCO3, 1 M NaCl,
steam-activated serpentine
Direct aqueous carbonation
2005; Stolaroff et al. 2005; Rodrigues and Joekes 2011).

heat-activated feedstock
Cement industries have large amounts of cement waste in

HCl/0.1 N NaOH
the form of cement kiln dust (CKD) and cement bypass dust
Direct carbonation
(CBD). In fact, for every 100 tonnes cement produced, 15–

20 tonnes of CKD is generated (van Oss and Padovani 2003).
Solution
Cement waste has very fine particles and high CaO content
(20–60%), making it highly reactive. Usually, CKD contains
38–48% CaO, but a fair portion of it is already carbonated as it
contains 46–57% of CaCO3 (Huntzinger 2009; Sanna et al.
15 mg/mL
15% solid
2014). CBD, however, has lesser quantities of carbonates than

50 mL/g
CKD. Hence, they have a substantial propensity to hold CO2

1 g/g
L/S
12
(0.5 tonne CO2 per tonne CBD) (Gunning et al. 2009).

5
1
Annually, CKD can hold approximately 42 Mt of CO2 which

Particle size
is 0.1% of CO2 produced (Bobicki et al. 2012). Using CKD as

feedstock for the carbonation process not only helps reduce
(μm)
< 75
< 38
< 75
< 37
~ 50
the CO2 levels in the atmosphere but also decreases its alka-
NA
linity, thereby making it less harmful to humans as it can

otherwise cause skin and eye irritations (Lange et al. 1996;
Pressure
Bin Shafique et al. 1998; Fernández Bertos et al. 2004a; Iizuka

(bar)
115
126
et al. 2004; Huijgen and Comans 2005; Huntzinger and

97
30
20
1
1
Eatmon 2009; Huntzinger et al. 2009). Additionally, it is ev-

Temperature
ident that carbonation helps improve the general cement

strength and regulate its corrosion properties (Papadakis
et al. 1991; Johannesson and Utgenannt 2001; Short et al.
(°C)
200
155
325
155
70
80
80
2001; Van Balen 2005; Monkman and Shao 2006). For ex-
Table 5 (continued)
ample, Teramura et al. (2000) produced building materials by

CO2-activated hardening process in which water was mixed
with cement waste in equal proportions. This mixture is then
Wollastonite
Wollastonite
Serpentine
Serpentine
Serpentine
Serpentine
moulded into bricks and hardened overnight at 4 bar CO2

Materials
Olivine
pressure resulting in 16.5% carbonation (Kashef-Haghighi

and Ghoshal 2010). Also, through the indirect aqueous
carbonation process, Katsuyama et al. (2005) and Iizuka et al. Australia, Swaziland, Serbia, France, Greece and Italy, asbes-
(2004) used cement waste and made pure CaCO3. Firstly, Ca tos tailings are still available from past mining activity. Hence,
is extracted from cement waste in solution form using CO2 at use of asbestos tailings as feedstock for mineral carbonation
30 bar pressure. Subsequently, CaCO3 is precipitated at 1 bar could prove useful in these countries (Gerdemann et al. 2007;
pressure. About 50% of Ca was extracted at 30 bar CO2 and O’Dell and Claassen 2009).
50 °C in 7 min (Iizuka et al. 2004). In fact, the rate at which the The use of either direct or indirect aqueous carbonation
conversion was made varied indirectly with pressure and di- with pre-treatment of the feedstock and increased levels of
rectly with temperature. The CaCO3 precipitate produced was pressure and temperature could help improve the
98% pure (Katsuyama et al. 2005). carbonation efficiency of the asbestos tailings. In an
Baciocchi et al. (2010a) found out that CaO and Ca(OH)2 experiment, Larachi et al. (2010) found out that at low pres-
present in cement waste reacted with CO2 in ambient condi- sures of CO2, 0.5% carbonation occurred in 5 h at 375 °C in a
tions, causing a significant amount of Ca to dissolve at a rate humid environment. It is also found out that pre-treatment of
considered quick enough to be used for manufacturing. An the tailings increases the reaction rate. By studying the natural
experiment was conducted by Shtepenko et al. (2006), in weathering of old tailing piles, Wilson et al. (2009) observed
Portland cement where humidified cement waste (L/S = that carbonation of chrysolite asbestos occurred at a rate of
0.1 L/kg) was carbonated with 100% CO2 at 2 bar pressure 0.3% per year. Moreover, bioleaching and decreasing the par-
for 1 h. The experiment yielded 370 g CO2/kg residue (i.e. a ticle size of the tailings greatly improved the efficiency of
carbonation efficiency of 76%). carbonation (Chiang et al. 2013). Nevertheless, more research
is ought to be conducted to determine the levels of risk asso-
Mining and mineral processing wastes ciated with handling old asbestos tailings.
Using mine tailings or mineral processing wastes of alkaline Nickel tailings Nickel tailings contain large quantities of MgO
minerals for carbonation eliminates the costs and environmen- (40%). In spite of the high costs involved in using nickel
tal hazards involved in mining when minerals are used directly tailings in CO2 sequestration, research shows that the use of
for the carbonation process (Rahmani 2018). Besides, mineral new technologies to integrate the mining and CO2 sequestra-
processing wastes are already in the form of finely ground tion makes usage of nickel tailings as feedstock for mineral
particles, making them well suited for use as feedstock in carbonation viable (Hitch et al. 2010). Using ultramafic nickel
mineral carbonation processes (Wilson et al. 2009; Larachi deposits in mineral carbonation also helps stabilize the chrys-
et al. 2010; Power et al. 2010). Mine tailings produced in olite asbestos present in them, thereby reducing the environ-
asbestos, serpentine, dunite and serpentinite sites can be used mental impact (Gerdemann et al. 2007). According to Teir
in mineral carbonation (Wilson et al. 2009; Power et al. 2010). et al. (2007b, 2009), Mg extracted from nickel tailing using
Also, residues such as red mud and bauxite from aluminum HCl and HNO3 acids was carbonated with an efficiency of
manufacturing sites can be used in carbon sequestration to 94% with a projected cost of $600–1600 per tonne CO2
improve their properties and make them suitable for reuse (Larachi et al. 2010). Therefore, further developments need
and safe landfilling (Bonenfant et al. 2008a; Sahu et al. to be made in the integration of mining and carbonation pro-
2010; Yadav et al. 2010; Bobicki et al. 2012). cess using nickel tailings to help regulate the cost.
Asbestos tailings Despite the fact that asbestos tailings have Red mud
been used in mineral carbonation for quite some time, very
little research has been done in recent years (Goff and Lackner Alumina manufacturing residues, also known as red mud,
1998). This is probably due to the hazards involved in work- have also been studied for their carbon sequestration capacity
ing with asbestos tailings; 4 Mt of asbestos is produced glob- (Bonenfant et al. 2008a; Johnston et al. 2010). Red mud is
ally, and for every tonne produced, 20 tonnes of tailings is highly alkaline in nature (pH > 13). It contains compounds
generated. With proper consideration, these tailings would such as Al2O3 (10–20%), CaO (2–8%), SiO2 (3–50%), TiO2
make a very effective source for mineral carbonation due to (trace–10%) and Fe2O3 (30–60%) (Sahu et al. 2010); 70 Mt of
the high levels of MgO (~ 40%) present in them. Furthermore, red mud is manufactured every year as for every tonne of
the use of asbestos tailings in mineral carbonation would help alumina produced; about 1 to 1.5 tonne of red mud is gener-
in remediation of the asbestos tailings that pose considerable ated (Dilmore et al. 2008; Yadav et al. 2010). According to
health hazards (Gerdemann et al. 2007). Countries such as research, red mud can hold up to 0.01% of CO2 emissions
Russia, Zimbabwe, Kazakhstan and Brazil still undertake as- from fossil fuels globally, assuming they have a 5% CO2
bestos mining though, in most other places, asbestos mining uptake. This translates to 3.5 Mt of CO2 every year. Like
has been stopped due to associated health hazards. Even in asbestos tailings, red mud poses a threat to living organisms,
places, where asbestos mining has ceased, such as the USA, thus making it difficult to store (Bonenfant et al. 2008a;
Dilmore et al. 2008). However, carbonation of red mud de- ash and lime is extremely hazardous, owing to high levels of
creases its toxicity and mitigates the liability associated with lime, soluble salts and volatile toxic heavy metals (Fernández
its storage. The carbonated red mud also has a wide range of Bertos et al. 2004a; Li et al. 2007). Carbonation of municipal
useful applications such as in soil amendments, sewage treat- solid waste incinerator (MSWI) ash helps in stabilizing it be-
ment, brick and tile production, fertilizer additives and cement fore putting it into reuse or being sent for landfilling as it limits
industries. The carbon sequestration capacity of red mud is heavy metal mobility and also aids in CO2 sequestration. The
limited though (Bonenfant et al. 2008a). small particle size of MSWI ash, high CaO concentration and
The direct aqueous carbonation of red mud was investigat- proximity to CO2 sources are other factors that make MSWI
ed under low pressure and ambient temperature conditions ash favourable for CO2 sequestration (Fernández Bertos et al.
(Bonenfant et al. 2008a; Sahu et al. 2010; Yadav et al. 2004a; Li et al. 2007).
2010). According to Bonenfant et al. (2008a), red mud se-
questers up to 40 g CO2/kg from slurries with L/S = 10 kg/kg MSWI BA Since BA is considered to be non-hazardous, it is
at 20 °C. This process achieved complete carbonation of the used in various ways as a recycled material such as in road and
hydroxides of both Na and Ca elements in the residue in 24 h pavement constructions (Costa 2006). It contains a mixture of
(Bonenfant et al. 2008a). Due to high solubility, Na2CO3 and oxides, silicates (SiO2, Ca2Al[AlSiO7]), carbonates (CaCO3),
NaHCO3, the main carbonation products from red mud, have sulfates (Ca 6 A l2 (SO 4 ) 3 (OH) 12 ·26H 2 O, CaSO 4 , CaSO 4 ·
a lesser storage permanency compared to Ca–Mg carbonates 2H2O), Fe2O3, Fe3O4 hydroxide Ca(OH)2 and chlorides
(Sahu et al. 2010). Therefore, red mud is often mixed with (Costa 2006; Costa et al. 2007; Sanna et al. 2014). It also
brine before carbonation to increase the permanency of CO2 contains traces of Sn, Ba, Mn, Cr, Ni, Co, Sb and V
storage (Dilmore et al. 2008; Johnston et al. 2010). Though (Hjelmar 1996). Volatile elements such as Cd, Hg, As, Zn
both methods of carbonation are successful in stabilizing red and Pb that are prevalent in APC in high concentrations are
mud with regard to its environmental impact, use of brine found only as trace elements in BA. BA has uniform and fine
greatly helps in enhancing the permanency of the sequestered particle size, high specific surface area and high porosity due
CO2. The natural weathering process of historically generated to emission of gas from the material during combustion.
red mud, which is about 6 Mt per year, sequesters only 100 Mt MSWI BA has a relatively high alkalinity of 9.5 to 11.5 pH,
of CO2 (Si et al. 2013). However, the use of technological but the significantly low levels of Ca and Mg make BA less
advancements helps sequester an additional 6 Mt of CO2 be- efficient in terms of CO2 sequestration capacity with a CO2
sides remediating the red mud (Si et al. 2013). uptake of just 3.0 to 6.5 wt% (Fernández Bertos et al. 2004a;
Rendek et al. 2006; Costa et al. 2007; Gunning et al. 2010).
Waste ash However, Baciocchi et al. (2010b) found CO2 uptake range
between 4 and 14% depending on particle size. Despite this
Municipal solid waste ash, oil shale ash, coal fly ash, paper disadvantage, MSWI BA is still used in the carbonation pro-
mill ash, de-inked ash and other industrial combustion ashes cess as it helps chemically stabilize heavy metals such as Pb,
contain varying amounts of CaO and are hence suitable for Zn, Mo, Cu and Cd and limit their leaching activity as well as
CO2 sequestration (Pérez-López et al. 2008; Reynolds et al. improve their engineering properties (Meima and Comans
2014). However, the efficiency of CO2 sequestration from 1997, 1999; Meima et al. 2002; Chimenos et al. 2003;
waste ashes is considerably lower than that from other alkaline Fernández Bertos et al. 2004a; Polettini and Pomi 2004; Van
residues. CO2 sequestration from waste ashes offers certain Gerven et al. 2005; Rendek et al. 2006; Costa et al. 2007;
advantages such as proximity to CO2 sources and no require- Bobicki et al. 2012).
ment of comminution due to their small particle size (Ji et al.
2018; Li and Li 2018; Liu et al. 2018b; Yu et al. 2019). APC residues This residue contains unreacted lime, fly ash and
unburned carbon. Through the process of flue gas treatment,
Municipal solid waste incinerator ash Production of municipal APC slag is formed. Major crystalline phases present in the
solid waste (MSW) in the world is increasing at an alarming APC residues are Ca(OH)2 silicates, ammonium silicates,
rate. Even though incineration is deployed industrially for CaSO4 and salts (Bodénan and Deniard 2003; Fernández
disposal of MSW, where recycling or reuse is impossible Bertos et al. 2004a; Costa 2006). APC residues have high
(Fernández Bertos et al. 2004a; Li et al. 2007; Wang et al. alkalinity (pH > 12) due to the presence of lime. It also con-
2010), it still leaves behind solid residues such as APC tains a high concentration of volatile heavy metals such as Zn,
(20%) and bottom ash (BA) (80%) (Rendek et al. 2006). BA Pb, As, Cd, Hg, Cr, Ni and Cu, making it environmentally
contains slag, glass, ceramics, metals and other non- hazardous (Hjelmar 1996; Fernández Bertos et al. 2004a;
combustible organic compounds and is considered a non- Bobicki et al. 2012; Sanna et al. 2012a).
hazardous waste (Fernández Bertos et al. 2004a; Li et al. Various methods such as thermal processing, physical–
2007). However, APC which includes unburned carbon, fly chemical separation and chemical stabilization are used to
stabilize APC residues to mitigate its adverse effects on the The sequestration potential of coal ash depends on the
environment (Sabbas et al. 2003; Quina et al. 2008). chemical composition of coal (Wu et al. 2011). Coal fly ash
Carbonation of APC residues also reduces alkaline levels of is fine in texture (10–15 μm). Bituminous coal fly ash has a
the residue to acceptable limit (pH < 9.5) (Ecke 2003; CO 2 sequestration potential of low ~ 9 wt% (Montes-
Fernández Bertos et al. 2004c). In addition, the high compo- Hernandez et al. 2009; Sanna et al. 2012a). However, in lig-
sition of Ca(OH)2, large surface area and porosity make APC nite coal and oil shale ashes that are rich in Ca elements, the
residues suitable for CO2 sequestration (Fernández Bertos carbon uptake can go up to 43–49% (Back et al. 2008; Uibu
et al. 2004b; Baciocchi et al. 2006, 2009a; Sun et al. 2008; et al. 2011). In addition, coal fly ash holds recrystallized min-
Sanna et al. 2012a). Contrary to MSWI BA, APC residue erals such as mullite (3Al2O32SiO2), CaO, cristobalite (SiO2),
carbonation is more desirable as the main reactive species in quartz (SiO2) and amorphous aluminosilicate glass matrix
the residue includes easily reacting CaClOH and Ca(OH)2 (SixAlyOz) and also contains unburned carbon in varying
(Fernández Bertos et al. 2004a). APC residues were carbon- quantities (Sanna et al. 2012a).
ated using both the direct gas–solid carbonation and the aque- Substantial research on carbonation of coal fly ash has been
ous carbonation methods with a CO2 uptake in the range of 7 done primarily on direct routes of aqueous carbonations with
to 12–13% (Fernández Bertos et al. 2004a; Baciocchi et al. water (Back et al. 2008; Montes-Hernandez et al. 2009; Uibu
2006). From the study, it is apparent that APC consumption of et al. 2010; Muriithi et al. 2013) and brine (Soong et al. 2006;
CO2 is greater than that of other MSW combustion wastes. Nyambura et al. 2011) as the reaction medium or by natural
Furthermore, changing parameters such as temperature, pres- weathering over a long duration (Uibu et al. 2009; Muriithi
sure, concentration levels and the particle size of APC residue et al. 2013). Under these conditions, it is estimated that the
impact its CO2 uptake abilities (Fernández Bertos et al. 2004a; process has 5% CO2 sequestration capability that could uptake
Prigiobbe et al. 2009d). 0.25% of CO 2 produced from coal-fired power plants
(Montes-Hernandez et al. 2009; Bobicki et al. 2012; Sanna
Coal ash Coal-based power plants contribute greatly towards et al. 2012a).
emission of CO2 in the atmosphere. Power plants running on
coal generate 40% of total global electricity (Montes-Hernandez Oil shale ash About 2.8 trillion barrels of oil in oil shale could
et al. 2009; Bobicki et al. 2012; Sanna et al. 2012a). During be produced (Külaots et al. 2010). This is a low-grade carbo-
power generation, coal combustion generates different types of naceous fossil fuel that exists in fine-grained sedimentary rock
coal ash such as bottom ash, fly ash, boiler slag and clinker form (Külaots et al. 2010; Uibu et al. 2010). Oil shale com-
which accounts for 5–20 wt% of the burnt coal. Fly ash and bustion produces a high ash content of 45 to 48% (Mõtlep
bottom ash are the major coal ash accounting for 85–95 wt% et al. 2010). Since oil shale ash has high levels of lime con-
and 5–15 wt% of the total ash produced, respectively (Yao et al. centration (20–25%) and is close to CO2 emission sources,
2015). Currently, approximately 600 Mt of coal ash is annually they are suitable for CO2 sequestration (Uibu et al. 2010).
produced worldwide (Ahmaruzzaman 2010). Oil shale ash is extremely alkaline in nature and similar to
The use of coal ash includes nutrients for plants; construc- coal fly ash and MSWI ash and has large amounts of heavy
tion of embankments, roads and structural fills; production of metals, unburned polycyclic aromatic hydrocarbons and phe-
building materials (concrete, cement and concrete-admixed nols, making it environmentally hazardous (Külaots et al.
products); synthesis of precipitated silica, zeolite and alum; 2010). Carbonation of oil shale ash also mitigates its potential
and use as an adsorbent to remove toxic ions and organic environmental hazards.
materials from wastewater and cleaning flue gas
(Ahmaruzzaman 2010). Alkaline paper mill waste
However, coal ash is hazardous to the environment as it
contains a high concentration of toxic heavy metals. Of the Production of cellulose pulp used in paper manufacturing
total coal fly ash produced, 30% of it is utilized effectively leads to the generation of alkaline paper mill wastes
while the rest is disposed of as landfill, causing damage to the (APMWs). These wastes have high CaO content of 45–80%
environment (Rostami and Brendley 2003; Ahmaruzzaman and hence suitable for carbonation (Pérez-López et al. 2008;
2010; Sanna et al. 2012a). This, however, can be better uti- Gunning et al. 2009). Simultaneously, the paper mill produces
lized in CO2 sequestration processes due to its close proximity CO2 in lime kiln as well as the recovery boiler that can be used
to CO2 emission sources and the presence of free lime. In for APMW CO2 sequestration (Nurmesniemi et al. 2008). The
addition, fly ash particles are very fine particles, chemically resulting CaCO3 from this process could be reused in the plant
reactive, with huge surface area for adsorption and minerali- or sold as a by-product (Pérez-López et al. 2008; Bobicki et al.
zation of CO2. This would help mitigate the environmental 2012). Pérez-López et al. (2008) found APMW which con-
impact of the resultant residue. The carbonation potential of tains 83.2% CaO could uptake 218 g CO2/kg paper waste at
coal fly ash is comparable to that of MSWI ash. 30 °C and atmospheric pressure in 2 h using the direct aqueous
carbonation method. An average-sized cellulose pulp industry For cost evaluation of mineral carbonation, the National
has estimated a CO2 sequestration capacity of 15,000 tonnes Energy Technology Laboratory (NETL) carried out extensive
of CO2 (Pérez-López et al. 2008). It was also determined that research by selecting seven regions in the USA with large
APMW is highly desired for CO2 sequestration as it has a amounts of ultramafic ores and CO2 (O’Connor et al. 2005;
higher reaction rate irrespective of temperature and pressure Gerdemann et al. 2007). For these regions, sequestration costs
conditions and also offers a high sequestration capacity with a feedstock activation step were calculated. The lowest
(Pérez-López et al. 2008). costs were $54/tonne CO2, $64/tonne CO2 and $78/tonne CO2
with olivine, wollastonite and serpentine as feedstocks, re-
spectively. However, by taking the additional energy costs
associated with CO2 mineralization into account, the carbon-
Sequestration cost ation costs in terms of net CO2 avoided were $71/tonne CO2,
$81/tonne CO2 and $112/tonne CO2, respectively (O’Connor
The cost of equipment used and operational cost for CO2 et al. 2005; Gerdemann et al. 2007).
capture are crucial to determine the overall cost of sequestra- Huijgen et al. (2006a) investigated direct carbonation of
tion. The capture cost of CO2 in an integrated gasification wollastonite in distilled water. On the basis of process simu-
combined cycle (IGCC) power plant having an 85% CO2 lation (Aspen), 75% conversion in 15 min at 200 °C and
capture efficiency was determined to be $15/tonne. In situ 20 bar CO2 partial pressure was obtained at an estimated cost
CO2 sequestration requires transferring the captured CO2 to of $102/tonne CO2, which included fixed costs, variable costs
an appropriate storage site (IPCC 2005). The transportation and depreciation of investments. Most of the expenses were
cost of transferring the sequestered CO2 through pipelines is linked with feedstock and consumption of power for grinding
determined on the basis of the following factors: (i) flow rate, and compression, which accounted for $54/tonne and $26/
(ii) transportation type (onshore/offshore) and (iii) distance. tonne CO2 sequestered, respectively (Huijgen et al. 2007).
For a distance of 250 km, the cost of CO2 transportation Huijgen et al. (2007) suggested focusing on carbonation de-
through pipelines is determined to be $1 to $8/tonne CO2 gree owing to the high cost of wollastonite mineral and its
(Kienlen 1954; IPCC 2005). The in situ storage cost for CO2 required L/S ratio. In order to reduce the overall sequestration
in saline formations and depleted oil and gas sites is found to costs, it is recommended to integrate the mineral carbonation
be $0.5 to $8.0/tonne CO2, with a monitoring cost of $0.1 to with capture of CO2.
$0.3/tonne CO2 (Kienlen 1954; IPCC 2005). Similarly, for in Additionally, commercial benefits such as remediation of
situ ocean storage at a depth of 3000 m, the storage cost of hazardous waste like steel slags and ashes from power plants,
CO2 is found to be $5 to $30/tonne CO2 (Kienlen 1954; IPCC production of value-added products for use in construction
2005). industry and feedstock for existing processes can be
When in situ CO2 sequestration is not feasible due to the achieved by carbonation of industrial wastes. This leads to
unavailability of suitable geological sites or the amount of an overall cost reduction, thus making the process
CO2 sequestration is limited, expensive ex situ CO2 seques- industrially feasible. Stolaroff et al. (2005) studied an indirect
tration which costs about $50 to $300 per tonne CO2 is sug- route of carbonation process, which involved the dissolution
gested. Cost of CO2 sequestration is highly correlated to plant and carbonation of the contents of concrete waste or steel slag
size, operating conditions, feedstock pre-treatment, additives in water with atmospheric CO2. In this process, dissolution of
and separation/disposal of the reaction products. Also, addi- Ca(OH)2 and CaO from the alkaline solids is achieved by
tional costs are attributed to mining, milling, crushing and spraying an aqueous solution on a slag bed or concrete waste.
transportation of mineral ores. This is estimated to be $8/tonne The saturated solution absorbs CO2 from the air, producing
of mineral ore processed (Gielen 2003). CaCO3 that precipitates and facilitates further dissolution of
Direct aqueous mineral carbonation route is found to be the Ca(OH)2 and CaO. The expenditure for this route was calcu-
most efficient method for CO2 sequestration in ex situ condi- lated to be $8/tonne CO2 sequestered, which excluded trans-
tions (Lackner 2003; Huijgen 2007). This is the only carbon- portation cost of the slag. On the contrary, the use of steel-
ation method that has undergone an elaborate economic and making slag as a raw material causes a considerable rise in
energy evaluation (O’Connor et al. 2004, 2005). Though the total cost to $25/tonne CO2 sequestered, assuming a market
process provides a high degree of carbonation at acceptable price of $8/tonne of steel slag (Stolaroff et al. 2005).
reaction rates, it is still quite expensive for large-scale appli- Expensive CO2 sequestration processes could be made
cations with costs ranging from $40 to 80/tonne CO2 miner- economical by upgrading a waste product into a high-valued
alized (including the utilization of energy) (IPCC 2005). The commercial product. Katsuyama et al. (2005) and Iizuka et al.
costs are exorbitant considering it costs only $0.4 to $6.0/ (2004) extracted Ca from waste cement at a greater pressure of
tonne for CO2 stored geologically (Huijgen et al. 2005a; CO2 through indirect aqueous carbonation of pulverized waste
IPCC 2005). cement. Next, CaCO3 precipitation from the reaction mixture
was achieved at low CO2 pressures to produce pure CaCO3 (≈ geological sequestration if the capture and mineral CO2 se-
98% purity). Estimated cost for CaCO3 production was $136/ questration processes are integrated. Furthermore, cheaper
tonne which is significantly lesser than the market price of feedstock (such as industrial wastes) or profitable usage of
$200 to $350/tonne (Katsuyama et al. 2005). Potential profits the products procured, as in the raw materials used in con-
could be increased substantially if CaCO3 is purified to ultra- struction could entail lower expenditures of sequestration
high purity (> 99%). Katsuyama et al. (2005) estimated a pro- (Stolaroff et al. 2005). An economical and environmentally
duction cost of $323/m3 for ultrapure CaCO3, whereas its friendly product application could remarkably improve world-
market price is around $10,000/tonne. wide application and lower the sequestration costs. For in-
Direct carbonation process of red mud at ambient temper- stance, the chemical stability of carbonated red mud could
atures and pressures was studied (Bonenfant et al. 2008a; be utilized in a wide range of industries, including brick and
Sahu et al. 2010; Yadav et al. 2010), and CO2 sequestration tile industry, cement production, fertilizer production, treat-
costs were estimated to be $147/tonne CO2 (Sahu et al. 2010). ment of wastewater and plastics industry (Bonenfant et al.
A pilot-scale study of mineral carbonation process was 2008a). Developing appropriate large-scale continuous reac-
undertaken by reacting coal fly ash and flue gases in a fluid tors and application of different additives to increase the dis-
bed reactor. This was undertaken in an electric power plant, solution reaction could result in monetary savings. Additives
which generated energy from the combustion of coal at Point applied, if any, should be capable of complete regeneration
of Rocks, USA. Assuming a sequestration capacity of 0.1 to and recycling. In addition, for a complete assessment of the
0.2 tonne CO2/tonne coal fly ash, the preliminary estimation silicate amount and their occurrence in ores that could be
cost was $11 to $21/tonne CO2 for a 90% CO2 uptake (Reddy economically recovered for CO2 mineral sequestration, a
et al. 2011). It has been estimated that in coal-fired power more comprehensible investigation of the possible capacity
plants, coal fly ash having 5% capacity for average CO2 se- of mineral sequestration of CO2 is essential. An important step
questration could sequester 0.25% of CO2 emissions (Montes- in the carbonation of ores is the surface activation of the min-
Hernandez et al. 2009; Bobicki et al. 2012; Sanna et al. eral for better yields of carbonation. It is accomplished by the
2012a). application of numerous physical pre-treatment procedures,
The process of indirect aqueous carbonation could be im- namely reduction in size, magnetic separation and heat and
proved using a number of chemicals, such as HCl, HNO3, steam activation (O’Connor et al. 2005). Chemical pre-
CH3COOH and NaOH at a cost of $600 to $4500/tonne treatment methods (Maroto-Valer et al. 2005) applied on ser-
CO2 without regeneration. Newall et al. (2000) examined an pentine consisting of H2SO4 were effective in increasing the
HCl extraction route and inferred that this approach was less surface area from 8 to 330 m2/g.
worthy owing to the calculated cost of $179/tonne CO2 Table 6 summarizes the cost of CO2 sequestration using
avoided. The disadvantages of the method were the expendi- different sequestration methods.
ture related to the utilization of HCl (that is, in the preparation
and demand of materials that were corrosion resistant) and the
utilization of energy during the evaporation of water. In this Utilization of products
process, the consumption of energy during the process of de-
hydration and crystallization exceeded the generation of ener- Solid waste residues such as MSW are generally disposed by
gy in the power-generating station that yielded CO2 by a factor the following methods: landfill (82%), composting or
of 4 (Newall et al. 2000). Teir et al. (2009) utilized HCl/HNO3 recycling (11%) and treatment with heat (7%) (Fernández
for feedstock dissolution and NaOH for precipitation. They Bertos et al. 2004a). In contrast, steelmaking slag can be
concluded that regeneration of the chemicals used emitted reused as a civil engineering aggregate owing to its excellent
2.6 to 3.5 times the quantity of CO2 which was generated in engineering properties (Geiseler 1996; De Windt et al. 2011).
the process of carbonation (Teir et al. 2009; Eloneva 2010). Extensive studies have been carried out to explore the poten-
Using the CH3COOH route, PCC of high purity could be tial use of steelmaking slag, as an alkaline filler in paper mak-
produced at a cost of $1990/tonne CaCO3 (Eloneva 2010). ing; as an aggregate in the manufacture of asphalt concrete
Based on a rough estimation of energy costs, which excluded (Lim et al. 2010), ceramic tiles, bricks (El-Mahllawy 2008)
other variable and investment costs, the sequestration costs and bituminous paving mixtures (Sorlini et al. 2012); and as a
were estimated to be $21/tonne CO2 avoided (Kakizawa replacement for either cement or sand. Other reuse options
et al. 2001; Huijgen and Comans 2003). explored for steelmaking slag are as a binder in substances
It was shown that direct aqueous mineral CO2 sequestra- based on cement (Fernández-Jimenez et al. 2006; Lim et al.
tion was feasible in terms of both energy and technology, but 2010; Zhang et al. 2011), conditioning of soil and amend-
it is still quite expensive to be competitive with other CO2 ments of land (Stolaroff et al. 2005). Similarly, various form
sequestration processes. However, mineral CO2 sequestration of fly ash also have applications in the construction industry as
could be competent economically in comparison with they are used as an additive in cement. As per Pozzolan
Table 6 Cost of different sequestration methods
Sequestration method Feedstock Cost $/tonne CO2 Remarks References
Geological
Storage 0.5–8.0 Monitoring cost is not included (IPCC 2005)
Monitoring 0.1–0.3 (IPCC 2005)
Ocean
Pipeline 6–31 100–500 km offshore distance and (IPCC 2005)
3000 m depth
Ship 12–16 100–500 km offshore distance and (IPCC 2005)
3000 m depth
Mineral 50–100 (IPCC 2005)
Wollastonite Direct aqueous carbonation (water) 91 $112/tonne CO2 avoided (Gerdemann et al. 2007)
Wollastonite Direct aqueous carbonation (water) 86 $102/tonne CO2 avoided. Both cases (Huijgen et al. 2007)
excludes CO2 capture cost
Wollastonite Indirect aqueous carbonation 63 Fixed cost: $9/tonne CO2 (Kakizawa et al. 2001)
(acetic acid) Variable cost: $54/tonne CO2
Olivine Direct aqueous carbonation 54 $78/tonne CO2 avoided (Gerdemann et al. 2007)
(0.64 M NaHCO3, 1 M NaCl)
Serpentine Direct aqueous carbonation 250 $309/tonne CO2 avoided (Gerdemann et al. 2007)
(0.64 M NaHCO3, 1 M NaCl)
Heat-treated serpentine
Mg silicate Direct carbonation (molten MgCl2) 63 Fixed cost: $11/tonne CO2 (Newall et al. 2000)
Variable cost: $52/tonne CO2
Mg silicate Indirect aqueous carbonation (HCl) 233 High cost for make-up chemicals (Newall et al. 2000)
and dehydration steps
Steel slag, Direct aqueous carbonation (water) 8 Capital, maintenance and operation (Stolaroff et al. 2005)
waste concrete cost included; transportation cost
excluded
Steel slag Direct aqueous carbonation (water) 64 $77/tonne CO2 avoided. Both cases (Huijgen et al. 2007)
excludes CO2 capture cost
Waste cement Indirect aqueous carbonation (water) 22.6 Considered CO2 separation and (Iizuka et al. 2004)
pressurizing cost, stirring,
pulverizing cost and revenue
generation by selling CaCO3.
Capital cost and maintenance cost
are not included
This article reports 1€ = 1$
reaction, the Al2O3 and SiO2 present in the fly ash react with and CKD decrease the leaching of Pb, Zn and Cu but show an
water and slaked lime from the Portland cement upon mixing increased leaching activity of Cd and Sb (Sanna et al. 2014).
together. This leads to the production of hydrates of calcium At present, quarry fines are widely used in mine reclama-
aluminate and calcium silicates, which increases the chemical tion (Kumar and Hudson 1992). Carbonated products also
resistance and strength of the cement considerably (Wee find a diverse set of applications as bulk fills in trenches and
2013). Hence, Portland fly ash cement finds application as a embankments, backfilling underground caverns, construction
concrete in the construction of dams. of landfills, remediation and improvement of soil and artificial
The benefits of steelmaking slag listed above are owing to soils and in other applications of general filling (Jones et al.
the formation of insoluble CaCO3 from compounds like CaO, 2009; Sanna et al. 2012b).
Ca(OH)3 and MgO present in the slag (Motz and Geiseler Currently, most carbonation processes are focused on pu-
2001) during the carbonation process. Moreover, carbonated rification of the precipitated Mg and Ca carbonated that in-
particles agglomerate and become coarser, thereby increasing creases their commercial value to boost the economic viability
their usefulness as of aggregates (Fernández Bertos et al. of the process (Lackner et al. 1997; Fagerlund et al. 2012;
2004c). Carbonation of minerals could also be employed to Sanna et al. 2013a). Research has also been carried out on
lower the mobility of toxic heavy metals present in wastes by the recovery of valuable metals such as Fe, Ni, Cr, Mn and
decreasing the pH levels and reduce the porosity through for- Al present in trace amounts in the ultramafic minerals such as
mation of crystals (Van Gerven et al. 2004; Rendek et al. in olivine and serpentine (Basile et al. 2010; Rajapaksha et al.
2006; Gunning et al. 2010). Carbonation reactions of MSW 2012; Assima et al. 2013).
The by-products in a carbonation reaction, namely Mg/Ca by obtaining iron oxides through carbonated products in a
carbonate, silica and iron oxides, are of commercial value that steel plant is approximately $3–4/tonne of CO2 seques-
helps in the economic viability of the process. Using indirect tered (Sanna et al. 2012b). Owing to the numerous quali-
carbonation methods enables the production of these by- ties of iron oxides, such as high strength in tinting and acid
products with greater than 90% purity (Wang and Maroto- resistance, they find application in synthetic pigments,
Valer 2011c; Sanna et al. 2012b) as this process enables the which includes ceramics, paints and porcelain (Jones
separation of different streams of precipitation products. Silica et al. 2009; Sanna et al. 2012b).
from the carbonate is expelled, followed by the separation of
iron oxide streams by direct precipitation or gravity concen-
tration and could be purified to an extent of 99% through
Future directions
electromagnetic and ultrasonic separations (Velinskii and
Gusev 2002). The amorphous nature of silica with a small
This study explored a number of carbonation methods, param-
mean particle diameter of about 1 to 30 mm leads to its high
eters that control the process and future potential applications
value in the construction industry as a replacement or filler in
of carbonated products. Various drawbacks related to mineral
pozzolanic cement (Sanna et al. 2012b).
carbonation still need to be addressed, such as resolving the
As per Nduagu et al. 2012under solid–solid phase, ammo-
slow rate of reactions, necessity of large amounts of feedstock,
nium sulfate could be utilized in the extraction of magnesium
decreasing the high overall cost of CO2 sequestration and
from serpentine. For conventional use in refractories and
reducing the huge energy requirements to accelerate the car-
fillers, magnesia is formed from around 98% of magnesite.
bonation reaction. Successful deployment of an economical
MgCO3 boards with high specific gravity, manufactured from
and environmentally friendly sequestration route, which has
magnesite, are also used in the construction industry.
marketable carbon neutral products, can significantly improve
However, this has only a limited market at present (Sanna
worldwide application and reduce sequestration costs.
et al. 2012b). According to Sanna et al. (2012b) and Teir
et al. (2005, 2009), strong acid and alkali can also be used to
produce hydromagnesite of high purity, which could be useful
in many industries. For instance, hydromagnesite is used as a Conclusion
fire retardant (Teir et al. 2005, 2009; Wang and Maroto-Valer
2011c). Mineral carbonation is a reliable and durable CO2 storage
Calcite is manufactured by the carbonation of inorganic method. Huge quantities of Mg and Ca silicates and alka-
wastes and, occasionally, from wollastonite, which is a natural line wastes from industries are available across the globe,
rock. CaCO3 finds major use in the construction industry. could be subjected to carbonation to produce carbonates of
Moreover, it is also useful as a filler in the paper, pulp, plastic, Mg and Ca that are stable and cause little or no harm to
rubber and paint industries; as a coating pigment for giving their surroundings. However, mineral carbonation requires
opacity and brightness; and for obtaining better print quality stimulation which can be done by pre-treatment of feed-
owing to its excellent ink receptiveness (Eloneva et al. 2008b; stock and by making the reaction conditions optimal. The
Teir 2008). Many physical and chemical properties, such as current review analyses the various methods of carbon-
average size of particles, morphology, distribution, specific ation that utilize naturally occurring minerals as well as
surface area, polymorphism and chemical purity, contribute those that use industrial wastes as feedstock. Various op-
to the myriad uses of CaCO3 (Tai and Chen 1998). For in- erating conditions were analysed based on the application
stance, smoothness, shine and printing characteristics of paper method used and the feedstock type to arrive at different
are dependent on the particle size of CaCO3 (Domingo et al. process routes. The major limitation of large-scale deploy-
2006). ment of mineral carbonization is the consumption of car-
Silicate rocks rich in iron (e.g. serpentine (5–10%)) and bonation products generated in large quantities, high pro-
industrial wastes (e.g. steel slag (15–30%)) are best utilized cess cost and environmental issues. In order to lower ex-
in the extraction of iron oxides. This is followed by CO2 penditure and to address environmental hazards, the dis-
sequestration from the mineral that contains a lower quan- posal and reuse of the carbonation products were also de-
tity of iron. As suggested by O’Connor et al. (2005), the lineated. Also, to make the process industrially feasible,
mineralization of CO 2 by direct methods incorporated further scientific studies need to be made with a detailed
magnetic separation to exclude iron oxides present in the cost analysis to develop novel and efficient methods. In
crude mineral. The entire iron content was recovered as addition, there is a huge requirement for more reliable es-
iron oxide by the means of grinding and then magnetic timations of the effects of mining, transportation, process
separation, thereby excluding the need for any pre- and disposal resulting from carbonation owing to the in-
treatment with chemicals. The decrease in the expenditure creasing environmental concern.
Author contributions All authors contributed to the study conception and Baciocchi R, Polettini A, Pomi R et al (2006) CO2 Sequestration by
design. Literature search, data analysis and first draft of the manuscript Direct Gas - Solid Carbonation of Air Pollution Control (APC)
were written by Dr. Shashikant Yadav. Prof. Anurag Mehra critically Residues. Energy & Fuels 20:1933–1940
revised the work. All authors read and approved the final manuscript. Baciocchi R, Costa G, Polettini A et al (2009a) Comparison of different
reaction routes for carbonation of APC residues. Energy Procedia 1:
Funding This study is partially funded by a grant from the Consortium 4851–4858. https://doi.org/10.1016/j.egypro.2009.02.313
for Clean Coal Utilization (McDonnell Academy, St. Louis, USA). Baciocchi R, Costa G, Polettini A, Pomi R (2009b) Influence of particle
size on the carbonation of stainless steel slag for CO2 storage.
Data availability All data generated or analysed during this study are Energy Procedia 1:4859–4866. https://doi.org/10.1016/j.egypro.
included in this published article. 2009.02.314
Baciocchi R, Costa G, Di Bartolomeo E et al (2010a) Carbonation of
stainless steel slag as a process for CO2 storage and slag valoriza-
Compliance with ethical standards tion. Waste and Biomass Valorization 1:467–477. https://doi.org/10.
1007/s12649-010-9047-1
Competing interests The authors declare that they have no competing Baciocchi R, Costa G, Lategano E et al (2010b) Accelerated carbonation
interests. of different size fractions of bottom ash from RDF incineration.
Waste Manag 30:1310–1317. https://doi.org/10.1016/j.wasman.
Ethical approval and consent to participate Not applicable 2009.11.027
Back M, Kuehn M, Stanjek H, Peiffer S (2008) Reactivity of alkaline
Consent for publication Not applicable lignite fly ashes towards CO2 in water. Environ Sci Technol 42:
4520–4526. https://doi.org/10.1021/es702760v
Baláž P, Turianicová E, Fabián M et al (2008) Structural changes in
olivine (Mg, Fe)2SiO4 mechanically activated in high-energy mills.
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Ex Situ Mineral Carbonation

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Environmental Science and Pollution Research (2021) 28:12202–12231

A review on ex situ mineral carbonation

Keywords CO2 sequestration . Mineral carbonation . Waste stabilization . Waste utilization

Fig. 1 Different CO2 sequestration routes

Table 1 Comparison of different CO2 sequestration routes

Storage types Benefits Drawbacks Potential, Gt

Geological Developed technology Threat of leakage 1800 (Shukla et al. 2010)

Fig. 2 Different mineral CO2 sequestration routes

2MgðOHÞClðlÞ þ nH2 OðlÞ→MgCl2 nH2 OðlÞ

Table 2 List of chemicals used

Natural magnesium silicates in soil amendment (Maroto-Valer et al. 2005). Theoretically,

Table 3 List of potential minerals investigated for mineral carbonation

Minerals Chemical formula References

Waste materials Classification References

Biomass ash (Gunning et al. 2010)

BF slag 25 3 0.125 mL/g Wet carbonation 24 3 9 (Johnson 2000)

Coal FA 30 1 ~ 40 10 g/g Aqueous carbonation using DI water 18 26 82 (Montes-Hernandez et al.

(Maroto-Valer et al. 2005)

(Gerdemann et al. 2007)

(Huijgen et al. 2006a)

(Lin et al. 2008)

entire process through pH adjustment for dissolution and pre-

Cement manufacturing industries release considerably high

quantities of CO2 into the atmosphere which is about 5% of

Huntzinger et al. 2009). The total annual production of cement

(Schneider et al. 2011). Due to the availability of cement

wastes in abundance, ease of carbonation and potential for

Indirect carbonation using succinic acid

waste recycling, cement wastes presents a very suitable source

for mineral carbonation (Huijgen and Comans 2003;

Fernández Bertos et al. 2004c; IPCC 2005; Shtepenko et al.

2005; Stolaroff et al. 2005; Rodrigues and Joekes 2011).

Cement industries have large amounts of cement waste in

(CBD). In fact, for every 100 tonnes cement produced, 15–

2014). CBD, however, has lesser quantities of carbonates than

CKD. Hence, they have a substantial propensity to hold CO2

(0.5 tonne CO2 per tonne CBD) (Gunning et al. 2009).

Annually, CKD can hold approximately 42 Mt of CO2 which

is 0.1% of CO2 produced (Bobicki et al. 2012). Using CKD as

linity, thereby making it less harmful to humans as it can

Bin Shafique et al. 1998; Fernández Bertos et al. 2004a; Iizuka

et al. 2004; Huijgen and Comans 2005; Huntzinger and

Eatmon 2009; Huntzinger et al. 2009). Additionally, it is ev-

ident that carbonation helps improve the general cement

ample, Teramura et al. (2000) produced building materials by

moulded into bricks and hardened overnight at 4 bar CO2

pressure resulting in 16.5% carbonation (Kashef-Haghighi

Table 6 Cost of different sequestration methods

Sequestration method Feedstock Cost $/tonne CO2 Remarks References

This article reports 1€ = 1$

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