Renewable and Sustainable Energy Reviews 99 (2019) 220–233

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Renewable and Sustainable Energy Reviews

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

New classification of CO2 mineralization processes and economic evaluation T

Pavan Kumar Naraharisetti, Tze Yuen Yeo, Jie Bu
⁎

Institute of Chemical and Engineering Sciences, A⁎STAR (Agency for Science, Technology and Research), 1 Pesek Road, Jurong Island, Singapore 627833, Singapore

ARTICLE INFO ABSTRACT

Keywords: Ever increasing greenhouse gas emissions and global warming have brought greater focus to the areas of CO2
CO2 Mineralization capture and storage/utilization. Carbon mineralization is one CCS/U technology that can capture large quan-
Economic evaluation tities of CO2 and convert it into stable carbonate products that can be stored easily. Several CO2 mineralization
Direct aqueous carbonation processes have been proposed, however there are no commercial scale projects because there are still significant
CO2 capture
issues that need to be improved upon before commercialization can take place. In this work, we perform a review
Serpentine
of the available technologies and classify them into different groups. We have identified that a minimum of three
inputs are required to a CO2 mineralization process. These can be in the form of two energy inputs and one
chemical input or two chemical inputs and one energy input. When two forms of energy inputs are used, it is
invariable to use electricity which is a poor form of energy i.e., CO2 emissions per unit of useful energy is higher
than using heat as a form of energy. In view of this, we can qualitatively conclude that it may be worthwhile to
develop technologies that use two chemical inputs and heat as a choice of energy rather than use both heat and
electricity. It follows that the chemicals used must be regenerated using heat and not electricity. Further, we
evaluate the economics of the most well-known type of mineralization process to date, the Direct Aqueous
Carbonation (DAC) process, where the mineralization reaction takes place directly under aqueous conditions,
high pressures and temperatures.

1. Introduction be limited to 2C°. This amounts to a total capture of 120 G tonnes of

The use of energy is a vicious cycle. All the fuels that are used
around the world eventually contribute to release of heat to the en-
vironment. As the temperature of the environment increases, and as
societies become more developed, more and more energy is being used
to improve/maintain the quality of life. In view of this, the use of en-
ergy is expected to increase over the next few decades. While con-
sumers realise the importance of global warming, they have to strike a
balance between reducing the energy use and improving/maintaining
their quality of life and this certainly is a difficult choice for them to
make. It is the duty of industry to develop energy efficient equipment
and the duty of both the industry and government to try and develop
technologies and policies that mitigate global warming caused due to
increased use of energy and the release of heat thereof to the en-
vironment. Carbon dioxide is a greenhouse gas and it is important to
control/reduce its emissions in order to keep global warming in control.
CO2 emissions in the year 2014 were about 32.3 G tonnes/yr according
to the International Energy Agency (IEA) [1]. IEA has a goal of cap-
turing/storing 8 Gt/yr of CO2 by 2050 in order to maintain a 2DS (2°
temperature rise scenario) where average global temperatures rise can
CO2 between 2015 and 2050. If nothing is done and business is carried
out as usual, we may see 6DS (6° temperature rise scenario) mainly due
to 70% growth in energy demand by 2050. More recently [2], IEA
presented a comparison between the Intended Nationally Determined
Contributions (INDC) and 450 Scenario (which is a scenario where
there is a 50% chance of keeping temperature rise within 2C°). They
observed that there would be a gap of about 9 Gt/yr between INDC and
450 Scenario by the year 2030.
Clearly, CO2 emissions are one of the most important challenges
facing the future of the planet and it is important to address this now.
CO2 mineralization is considered as one of the safest means of capturing
and storing CO2 because the end products have a lower enthalpy of
formation than the raw materials. Further, the change in Gibbs free
energy of the process is negative and hence the products are stable.
Although the terms “CO2 mineralization” and “Mineral Carbonation”
are popular now a days, the process was earlier called as artificial rock
weathering where scientists have tried to improve the kinetics of a bio-
chemical process that occurs in nature. The overall reaction of rock
weathering of some of the mineral ores is [3–6]:
Olivine: Mg2SiO4 + 2CO2 → 2MgCO3 + SiO2 + 89 kJ/mol CO2

⁎
Corresponding author.
E-mail address: bu_jie@ices.a-star.edu.sg (J. Bu).

https://doi.org/10.1016/j.rser.2018.10.008
Received 14 November 2017; Received in revised form 13 August 2018; Accepted 4 October 2018
Available online 23 October 2018
1364-0321/ © 2018 Elsevier Ltd. All rights reserved.
P.K. Naraharisetti et al.
Serpentine: Mg3Si2O5(OH)4 + 3CO2 → 3MgCO3 + 2SiO2 + 2H2O +
64 kJ/mol CO2
Wollastonite: CaSiO3 + CO2 → CaCO3 + SiO2 + 90 kJ/mol CO2
Olivine and Serpentine reactions are related in that Olivine is a
precursor to Serpentine. In order to improve the kinetics of the process,
an external energy is required. This energy can be given to the system in
the form of electricity (incl. pressure), heat and/or chemical energy.
The use of energy by CO2 mineralization process liberates some CO2
and it is a necessary condition that the amount of this CO2 emitted by
the mineralization process is considerably less than the CO2 captured by
the CO2 mineralization process. When energy input is in the form of
pressure and heat and the mineral ores are reacted directly with carbon
dioxide, it is called direct carbonation. When chemicals are used for
acid leaching of the mineral ores and/or as a means of CO2 carrier, the
process is called indirect carbonation. Whenever chemicals are used, it
is important to regenerate them; else the demand for these chemicals
that are used for CO2 mineralization will far outstrip existing produc-
tion capacities and will add considerable costs to the CO2 mineraliza-
tion process in the form of new capital expenses, not to mention the
demand for resources to produce them, thus potentially causing a
bigger environmental problem.
CO2 mineralization relies on the use of mineral ores and about
3–4 tonnes of mineral ore (average 3.5 tonnes) is required to capture
one tonne of CO2. In order to capture 9 G tonnes/yr of CO2 a total of
about 32 G tonnes/yr of mineral ores are required. Although some CO2
mineralization technologies are focusing on the value of the products
produced, there is unlikely to be any market for the products once this
process is carried out on such a large scale as this. In view of this, the
only means of disposal of CO2 mineralization products is mine filling
and/or land reclamation from sea or even making man-made mountains
of mineral carbonates. Hence, CO2 mineralization is expected to be a
cost centre with hardly any revenue streams. In view of this, it is of
utmost importance to identify the important parameters that contribute
to higher costs and focus future research on areas that have the greatest
economic impact. Production cost involves both Operational cost
(OpEx) and Capital cost (CapEx); here we estimate the OpEx by using
our data in published literature [7] and also present the details of the
CapEx estimation.
2. Literature review
The literature in the area of CO2 mineralization is wide. A review of
various publications between 1990 and 2004 is available [5] and that
between 1990 and 2010 is also available [6]. According to these lit-
erature reviews, it was 1990 when CO2 carbonation using silicates was
mentioned for the first time [8]. However, disparate knowledge of how
to perform CO2 mineralization was available much earlier in the form of
extraction of magnesium from serpentine and forsterite [9,10] and re-
covery of acid through MgCl2 hydrolysis [11] where MgO is the by-
product. Further, knowledge of carbonation of calcium/magnesium
oxides was also available much earlier than 1990 and it was understood
that CaO reacts rapidly with CO2; however the reaction of CO2 with
MgO is slow. In these literature reviews [5,6], the traditional classifi-
cation into direct and indirect carbonation is presented in addition to
various sub-classifications. Further, they [5,6] have also reviewed the
various mineral ores and waste materials from mineral processing in-
dustries that are useful for mineral carbonation. This classification al-
lows us to get an understanding of the various technologies that are
available. In addition to these, there are several other publications in
the area of CO2 mineralization and these can broadly be grouped based
on the respective research group. In addition, a review of CO2 seques-
tration by mineral carbonation was done in [12,13] and that of pH-
swing process for mineral carbonation in particular was presented in
[14]. Briefly, these research groups are NETL [3,4,15], Comans & co-
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Renewable and Sustainable Energy Reviews 99 (2019) 220–233
workers [5,16,17], Zevenhoven & co-workers [18–25], Jie Bu and co-
workers [26–28], Shell Global Solutions, The Netherlands & colla-
borators [29,30], Maroto-Valer & co-workers [31–35], and some of the
others include [36–40]. While most of this research focussed on in-
organic acids, there are others who used organic acids. For the sake of
completeness a brief literature review of the application of organic
acids is presented later in this Section.
The literature reviews [5,6] provide an overview of the various
technologies that are available, but do not give us a clear understanding
of the various energy and chemical inputs to the process. In view of this,
review various different processes published and classify the various
technologies into different Groups based on the process route. This is a
preliminary classification and is not claimed to be complete; never-
theless it helps us identify a minimum number of input variables to the
CO2 mineralization process and provides some useful insights into how
researchers are developing new technologies. We classify the literature
into various groups and present the same in here. It must be mentioned
here that we do not include the use of organic acids (excluding acetic
acid) for acid leaching in this classification.
While much of the research is focused on the technology that is
being developed by the various research groups, detailed economic
evaluation of the process of CO2 mineralization is limited. In view of
this, we focus on the Direct Aqueous Carbonation (DAC) process which
is amongst the earliest of processes that is studied at pilot scale [3]. We
use this process as a basis for calculating the cost of CO2 mineralization
and identify critical parameters and unit operations that influence the
cost. Understanding the critical drivers of the costs helps focus future
research on areas that have the greatest economic impact. We also
present the methodology of the economic evaluation and evaluate the
DAC process.
Beyond the different research groups (mentioned earlier) that have
been active in the area over the last couple of decades, the topic has
been gaining importance and several publications have emerged in the
recent past. More recently, several publications have appeared in var-
ious journals and these have used raw materials such as mineral ores,
fly ash, and slag from the metals processing industries, concrete waste
and wastes from mineral processing facilities. For the sake of com-
pleteness, we review them here, but do not include the same in the
classification to keep the classification simple and tractable. A figure
showing the increased number of publications over the years is pre-
sented in Fig. 1. It must be mentioned here that this plot only covers
publications that are reviewed in this work and we can see that there is
increased interest in this topic in the last decade. It we observe closely,
we can see that the focus during the initial years was mostly on mineral
ores and there is increased interest during the last five years on using
industrial waste, concrete waste and fly ash.
Regeneration of the chemicals used in the mineralization process is
of paramount importance. This is needed in view of the scale of the
problem and amount of chemicals that would be required in addition to
mineral ores if regeneration is not performed. In view of this, research
was done on regeneration of the chemicals [41]. A new reactor for
studying three phase systems, with particular emphasis on application
to CO2 mineralization process has been developed [42]. Techno-eco-
nomic evaluation on CO2 mineralization using mining wastes and raw
flue gas has was performed in [43]. Influence of mechanical activation
on the CO2 mineralization of mining waste [44–46] was done along
with economic evaluation in [47]. It was observed that mechanical
activation of mine waste is better than grinding pure olivine. A detailed
mineralogical study was done [48] on serpentine to understand the
influence of characteristics of mineral on the mineralization process
while Wollastonite [49] and limestone carbonation [50] in supercritical
CO2 was revisited recently along with carbonation of magnesium sili-
cate [51]. An attribution based leaching carbonation process was stu-
died in [52]. A pH-swing process for mineral carbonation was presented
in [53–55].
Influence of molar ratio of metals in the ore on the extent of
P.K. Naraharisetti et al.
Fig. 1. Growth of publications (reports, journal papers and book chapters) in the area of CO2 mineralization (limited to publications reviewed in this work). Data for
the year 2018 is linearly extrapolated based on the number of publications until July 2018.
carbonation at atmospheric conditions was done in [56]. Phase equi-
librium studies on the magnesium/ammonium sulphate and water
ternary mixture was done in [57]. Separately, several pilot scale studies
using different types of reactors were conducted by various researchers
[58–62]. In [63], a mass balance analysis on three different processes to
understand which one is has potential for commercial application.
An interesting study on the CO2 sequestration of ultramafic milling
wastes in natural atmosphere has been conducted [64] and this study
tried to understand the mechanism of the same so as to get a view of the
implication of process in controlling atmospheric CO2. A similar study
was done using Nesquehonite ultramafic mining waste [65]. Mining
waste from lizardite and brucite [66] and Brazilian serpentinites [67]
were used in a study to analyse the leaching step. Magnetic separation
of serpentine mining residue followed by mineral carbonation was done
in [68]. Direct aqueous carbonation of waste slate was done in [69]
while, studies on the use of byproduct of mining includes the use of red
gypsum [70–72]. Research using other ores such as magnesite [73],
tholeiitic basalt [74] are also available in literature. Process simulation
of mineral carbonation of phosphogypsum was studied in [75,76].
Utilization of blast furnace/steel/metallurgical slags [77–91], gypsum
waste [92–95], concrete waste [90,96,97], fly ash [98–105], cement
kiln dust [79,106], ceramic brick [107], soda ash plant waste [108],
bauxite residue [109] and carbide slag [110,111] in mineral carbona-
tion was also studied by researchers. Some other interesting studies are
on the use of the byproducts of mineral carbonation in pozzolanic ce-
ment replacements [112] and use of mineralization products in con-
crete blocks [113], while others have studied the possibility of using
CO2 in curing of cement paste [114].
Acetic acid is one of the most common organic acids that has been
proposed for acid leaching of mineral ores. Formic acid, acetic acid and
lactic acid were used for acid leaching of Wollastonite and it was ob-
served that formic acid performed the best amongst them with 96%
leaching in three hour [115]. The yield of the leaching process was
about 85% for acetic and 90% for DL-lactic acid. Some researchers have
studied acid leaching using succinic acid and adipic acid [116] while
others [54,117–119] have used one or more of oxalic acid, citric acid,
ascorbic acid, and ethylenediaminetetraacetic acid (EDTA). However,
in these studies [54,115–121] the mineralization step was not per-
formed by the researchers. In addition to these organic acids, a mixture
of orthophosphoric acid, oxalic acid and EDTA was used by some [120]
while others [121] have used a mixture of sodium oxalate and sodium
citrate. An integrated CO2 capture mineralization using amines was
presented in [122]. Citrate additives were studied to understand the
mineralization process at the nanoscale in [123] while methanol was
used in [124]. Although the natural rock weathering process is affected
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Renewable and Sustainable Energy Reviews 99 (2019) 220–233
by various organic acids produced due to biological action, it is not
clear from these works [54,115–121] as to how the organic acids will
be regenerated when they are used in an industrial setting. Regenera-
tion of the acid used for leaching is of utmost importance in order to
keep the costs low especially when the target is to capture 9 G tonnes/yr
of CO2. In addition to organic acids and solvents, biological/enzyme
based methods were also used in the process of mineral carbonation
[125,126]. Carbonic Anhydrase was tried in [127] and a microbial
method was tried at an asbestos Mine [128].
3. Classification of CO2 mineralization technologies
It is important that the cost of a process is low in order to be able to
capture CO2/reduce global CO2 emissions on a large scale. Hence, it is
important to understand the processes in enough detail to be able to
quantify the main costs. In view of this, we perform a preliminary
classification of the literature into various groups in order see if there
are any patterns in the stoichiometry of the various processes exist. This
with a hope that future research can be focused on promising patterns.
In view of the large volume of publications that are available, to keep
the classification tractable, we consider only the most relevant litera-
ture up to the year 2015 for this classification as these form the basis for
much of the work that has appeared in the recent past.
3.1. Review of different processes
The literature that is cited in Table 1 (Process 1–13) mostly uses
inorganic chemicals. In order to group the different processes, we first
analyse the process route to identify the important factors that influ-
ence the process. These are related to the operating conditions and the
various chemicals that are used in the process. The operating conditions
are related to the different forms of energy that are used in the process.
These are also listed in Table 1. Energy is given to the process in the
form of electricity and heat. Here, we must note that electricity can be
used in two forms, for generation of pressure and for driving electro-
chemical reactions. Chemicals are used for acid leaching of mineral
ores, as a CO2 carrier, as a regenerating agent that can be regenerated
along with the products and sometimes as a buffer that aids mineral
digestion and carbonation. Table 1 shows the various technologies that
are classified into Groups A to F based on the important factors men-
tioned earlier. Next, we present the details these groups, briefly:
Group A: Processes 1–3 use pressure and temperature as a means to
achieve direct carbonation of the mineral ores. The temperature and
pressure vary in each of these processes; however, all use one chemical
or the other to expedite leaching of the mineral or as CO2 carrier or
 P.K. Naraharisetti et al.

Table 1
The Table shows the various technologies classified into different Groups from A to E.

Process Leaching agent CO2 carrier/mineralisation route Regenerating agent Recyclable Recyclable Major energy input Max. operating Reference Group
intermediate product conditions

1 – Buffer – – – Heat & Pressure T = 200 °C; [3,16,17] A

P = 150 bar
2 – NH4OH in place of Buffer – – – Heat & Pressure T = 160 °C; [37] A
P = 20 bar
3 CH3COOH in place of Buffer – – – – Pressure T = 80 °C; [19,39] A
P = 30 bar
4 HCl NaOH – – NaCl Electricity (Bi-polar T = 80 °C; P = 1 atm [145] B
membrane electro-dialyzer)
5 HNO3 (HCl may also be used) NaOH – – NaNO3 Electricity (Electrolysis) T = 70 °C; P = 1 atm [20] B*
6 HCl NH4OH NH4HSO4 – NH4Cl Heat T = 350 °C; [29] C
P = 1 atm

223
7 HCl NH4OH Mg(OH)2 – NH4Cl Heat T = 550 °C; Possible alternative C*
P = 1 atm to [146]
8 NH4HSO4 NH4OH – – (NH4)2SO4 Heat T = 300 °C; [31,32] D
P = 1 atm
9 (NH4)2SO4 – NH4OH MgSO4 – Heat & Pressure T = 550 °C; [21,22] D*
P = 35 bar
10 HCl – – MgCl2 – Heat & Pressure T = 450 °C; [36] E
P = 340 bar
11 CH3COONH4, NH4NO3 and/or NH3/pH swing – – – – T < 100 °C; P = 1 [18,38] F
NH4Cl atm
12 CH3COOH (Acetogenic bacteria CH4 generation (Methanogenic – – – – T < 100 °C; [125,126] F
creates a buffer via acid leaching) bacteria) P = 1 atm
13 Not applicable as CaO from fly ash Glucose as substrate for Yeast & – – – – T ~25 °C; P = 1 atm [40] F
is used Peptide CaCO3 precipitation

* Theoretical processes
Renewable and Sustainable Energy Reviews 99 (2019) 220–233
P.K. Naraharisetti et al.
both. The major energy inputs to these processes are due to the che-
micals (buffer or leaching agent), pressure and heat.
Group B: Processes 4 & 5 use an acid for leaching of the mineral ore
and a chemical base as a CO2 carrier. The salt that is produced is re-
generated in an electro-chemical process which occurs at reasonably
low temperature. These processes occur at atmospheric pressure and
the major energy inputs to these processes are due to the chemicals
(buffer or leaching agent) and electricity.
Group C: Processes 6 & 7 use an acid or salt for leaching of the
mineral ore and base as a CO2 carrier. In addition, a regenerating agent
such as ammonium sulphate or magnesium hydroxide is used to re-
generate the acid and base from the ammonium salt that is produced.
All reactions are carried out at atmospheric pressure and a maximum
temperature of between 300 °C and 550 °C is required to regenerate the
acid and base depending on the process. The major energy inputs to
these processes are thus chemicals and heat.
Group D: Processes 8 & 9 use ammonium (bi)sulphate as a mineral
leaching agent. This is in contrast and counter-intuitive to most of the
other processes that use acid or a buffer for acid leaching. Process 8 is
experimentally verified while Process 9 is a hypothetical process. Both
these processes require two chemical inputs and heat. However, Process
8 can be carried at atmospheric pressure whereas it is proposed that
Process 9 is performed at 35 bar.
Group E: Process 10 uses only one chemical for acid leaching and
carbonation is performed at high pressure. The intermediate is hydro-
lysed at high temperature to regenerate the acid. Overall, the process
uses one chemical input and heat and the operating pressure is atmo-
spheric.
Group F: Processes 11–13 are carried out at near to RTP. Process 11
uses a buffer while Process 12 uses acetogenic bacteria which produced
acetic acid for leaching of the ore. Carbonation is achieved via the use
of a pH swing (chemical action) or with the action of methanogenic
bacteria producing metal carbonate and methane. Further, the aceto-
genic bacterium requires a substrate that acts as an energy source to
grow and produce acetic acid. In Process 13 researchers have developed
an engineered yeast based CO2 mineralization process that occurs at
room temperature and pressure. The source of calcium is fly ash and
Glucose is used as a substrate to culture the yeast. Since these processes
are carried at RTP, we can expect that the kinetics are very slow, which
is in fact what was observed in the experiments.
Now that we have classified the works into six different groups, we
further try to find if there is any structure/logical similarity between
one process and the other in next Section.
3.2. Energy and chemical inputs of different groups (A to E)
From Table 2, we identify the use of different types of chemicals
that are used in a given Process Group A to E (Group F is neglected as it
corresponds to processes that are too slow to be viable at industrial
scale); they are salt, acid, base and/or regenerating agent. A salt may in
conjunction with an acid/base give a buffering action. Some ammo-
nium salts may give the buffering action without the involvement of an
acid/base (Process 2 & 3 in Table 1). Further, the type of energy input
Table 2
The Table shows the various Groups of technologies and the energy/chemical inputs required for each of the processes.
Chemical input Energy input
Salt/Buffer Acid Base Regenerating Agent Pressure
Group A Acid/Base/Buffer/Salt is required N Y
Group B N Y Y N N
Group C N Y Y Y N
Group D Y N Y N Y
Group E N Y N N Y
Renewable and Sustainable Energy Reviews 99 (2019) 220–233
that is required is also listed as Pressure, Heat and/or Electricity, where
electricity does not include the use of compressor for generating pres-
sure.
It can be seen from Table 2 that a minimum of three forms of “In-
puts” are required for a CO2 mineralization process; this can be a
combination of 1 Chemical Input and 2 Energy Inputs (Groups A & E) or
2 Chemical Inputs and 1 Energy Input (Groups B, C & D). We can fur-
ther classify the different Groups into Electricity based process (Group
B), Heat based process (Group C) and Electricity and Heat based pro-
cesses (Groups A, D & E). Pressure (generated by using electricity in a
compressor) and Electricity are poor forms of energy inputs to the
system as the power plant efficiency is usually 30–45%. Since the ef-
ficiency is low, CO2 emissions per unit energy output from a power
plant are higher. However, use of Heat has a thermal efficiency of
80–90% and CO2 emissions per unit energy output can be expected to
be comparatively lower. In view of this, we can possibly expect that
Electricity based processes will have a higher energy penalty and hence
a higher CO2 penalty compared to Heat based processes. However, a
detailed analysis and quantitative comparison of energy requirements
and CO2 emissions of the different processes is required for a better
understanding and this is beyond the scope of this paper. Energy pen-
alty and CO2 penalty of two processes are presented in [7].
Table 2 does not consider Group F which is a classification of slow
biological processes. It can be seen from this Group that when only two
inputs (Group F) are given to the system with hardly any energy input,
the speed of the reaction is compromised. Hence, we can qualitatively
conclude that three inputs are required for the CO2 mineralization
process in order to improve the kinetics and it is probably best to use
Heat as the preferred mode of energy input. We must note hear that the
use of electricity as an energy input to CO2 mineralization can bring
undue pressure on existing power plants and it would become necessary
to build dedicated power plants for CO2 mineralization leading to an
increase in capital costs. Alternatively, if power is used from an existing
power plant, then the net electricity available for sale reduces and this
leads to an increase in price of electricity for the consumer. Either way,
the use of electricity leads to a cost increase for one stakeholder or the
other. On the contrary, the use of heat involves simpler equipment such
as furnace and heat-exchange equipment which are potentially cheaper.
Further, from a safety point of view, high pressure equipment is in-
herently expensive compared to heat exchange equipment. In view of
this, if pressure is required for the process, then the operating condi-
tions must be optimized such the energy required for pressure is as low
as possible i.e., a low pressure heat-based process should be developed.
3.3. Future direction
It can be seen from the above discussion that a minimum of three
inputs are required to improve the kinetics of the process. Group F is an
exception and it requires two chemical inputs and this renders the
overall kinetics slow. In process 12, acetogenic and methanogenic
bacteria are used and this may be equated to two (bio)chemical actions.
In process 11 however, only ammonium chloride performs the action of
two chemicals, where the second is ammonia produced from the
Energy basis Energy efficiency (qualitative
assessment)
Heat Electricity (other than
pressure)
Y N Electricity & Heat Low
N Y Electricity Low
Y N Heat High
Y N Electricity & Heat Low
Y N Electricity & Heat Low
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P.K. Naraharisetti et al. Renewable and Sustainable Energy Reviews 99 (2019) 220–233

ammonium chloride reaction with mineral ore. In an another recent Table 4

publication [129], researchers have observed that it is possible to Comparison of economics of different processes – Reported values vs. iPEAD.
achieve 70% conversion of Olivine in 4 hrs and 90% conversion in less Source:Adapted from [54].
than 24 hrs at a temperature of 180 °C and 20 bar pressure. It must be No. Process Reference CapEx CapEx by Deviation
noted here that the slurry concentration is 9% which is much less than Reported (M iPEAD (M$)
the 30% concentration that the NETL process uses [3]. The CO2 and $)
energy penalty of processes [3] and [129] are presented in [7] and the
1 Natural gas [141] 513.1 640.3 + 25%
penalties for process [129] are much higher due to low slurry con- reforming
centration leading to higher heat requirement of heat more water. From 2 Lummus OCT [142] 159.3 174.1 + 9%
Group F and from [129] we can conclude that mild operating condi- 3 Biofine process [143] 50.7 45.9 − 10%
4 Gasoline from wood [144] 138.5 134.0 − 3%
tions such as low pressure requires dilute operating environment and
5 Biofuel production [140] 15.3 15.6 + 2%
leads to slower kinetics. – syngas cleaning
It can thus be concluded that existing processes are fast only when 6 Biofuel production [140] 102.8 94.9 − 8%
three inputs are given to the system. In ‘Nature’ the rock weathering – fuel synthesis
process occurs via the action of two complex (bio)chemical steps (si-
milar to Process 12) and it is knows that this is a slow process. Hence,
we may qualitatively conclude that the third input to the system “may one reactor and/or furnace and/or separator. In view of this, we can
be” necessary condition to improve the kinetics of the CO2 miner- qualitatively conclude that the CapEx of processes in Group C would be
alization/artificial rock weathering process; however exceptions do the highest amongst all the processes. This looks like a classic optimi-
exist. zation problem in chemical engineering wherein Group C potentially
An exception to this is that Wollastonite can be used in CO2 mi- has the lowest operational cost (and is most energy efficient) and is
neralization with only Heat and Pressure as inputs; a buffer is not re- potentially the most expensive in terms of CapEx. However, it must be
quired unlike Serpentine or Olivine [3,15]. Further, Wollastonite is a emphasised here that CO2 mineralization process is unlike other che-
relatively purer mineral in terms of Calcium content and other metal mical processes especially since energy efficiency directly influences
impurities are low in content. Further, it is comparatively soft mineral the amount of CO2 avoided and hence the CapEx, but in other chemical
ore and this helps in easy chemical reaction with only the use of processes energy efficiency has only an indirect and typically a smaller
Pressure and Temperature. It is thus clear that exceptions do exist and influence on CapEx. In view of this, we can qualitatively conclude that
the research community has largely focused on complex processes with it may be worthwhile to pursue CO2 mineralization processes that fit
three or more inputs. Now, it is for the research community to explore the overall scheme of Group C where no electricity is used. It would be
further on the availability of simple mineral ores along with chemical ideal if governments are charitable organization take the burden of
inputs that can be used in CO2 mineralization with the use of little or no higher CapEx but such policy research is beyond the scope of this work.
Heat and Pressure. It must be mentioned here that the maximum vo-
lume of low pressure reactors is 500 m3 while that of high pressure
4. Economic evaluation
reactors is 200 m3. Since cost of reactors is proportional to the 2/3rd
power of the volume, it is cheaper to use high volume reactors and thus
4.1. Integrated preliminary economic analysis and design (iPEAD)
chose low pressure processes.
methodology
From Table 2, we have seen that the qualitative assessment has
shown that Group C possibly consumes the least amount of energy
We have developed iPEAD, an in-house software tool, which is used
mainly because electricity is not used in these processes. However,
to make a quick economic assessment during early stage process design
three different chemicals are used in this Group. It is important to un-
by evaluating factors such as equipment costs, depreciation, and op-
derstand the effect of using more chemicals for the CO2 mineralization
erational costs such as raw material and utilities among others. It helps
process. In view of this, we have presented the detailed mechanism of
researchers visualize and identify problems present in the process by
the different groups is given in Table 3. We can see from Table 3 that
highlighting the most cost-intensive components in the entire process.
Group A has only one reaction step whereas Group C has the most the
In iPEAD, shortcut methods for sizing and costing various unit opera-
reaction steps that stand at 5. It is likely the each reaction step requires
tions are employed to get a quick estimate of CapEx and OpEx based on

Table 3
The Table shows the various technologies classified into different Groups from A to E and the reaction mechanism.
Group A Group B Group C Group D Group E

R1 Mg3Si2O5(OH)4 + 3CO2 Mg3Si2O5(OH)4 + 6HA
= 3MgCO3 + 2SiO2 + 2H2O = 3MgA2 + 2SiO2 + 5H2O
T > 100 °C; P > 40 bar T = 80 °C; P = 1 atm
R2 2MOH + CO2 = M2CO3 + H2O
T = 25 °C; P = 1 atm
R3 M2CO3 + MgA2 = MgCO3
+ 2MA
T = 25 °C; P = 1 atm
R4 MA + H2O + Heat/Electricity
= MOH + HA
T = 25 °C; P = 1 atm using
BMED
R5
Products are NOT separated Products are separated
Mg3Si2O5(OH)4 + 6HA
= 3MgA2 + 2SiO2 + 5H2O
T = 80 °C; P = 1 atm
2NH4OH + CO2 = (NH4)2CO3
+ H2O
T = 25 °C; P = 1 atm
(NH4)2CO3 + MgA2 = MgCO3
+ 2NH4A
T = 25 °C; P = 1 atm
NH4A + MOH/Salt = NH3
+ H2O + MA
T = 25 °C; P = 1 atm
MA + H2O + Heat = MOH
+ HA
T = 500 °C; P = 1 atm
Products are separated
Mg3Si2O5(OH)4 + 6NH4HSO4
= 3MgSO4 + 2SiO2 + 5H2O
+ 3(NH4)2SO4
T = 90 °C; P = 1 atm
NH4OH + CO2 = NH4HCO3
T = 10 °C; P = 1 atm
MgSO4 + NH4HCO3 + NH4OH
= MgCO3 + (NH4)2SO4
T = 80 °C; P = 1 atm
(NH4)2SO4 + H2O = NH4HSO4
+ NH4OH
T = 300 °C; P = 1 atm
Products are separated
Mg3Si2O5(OH)4 + 6HA
= 3MgA2 + 2SiO2 + 5H2O
T = 80 °C; P = 1 atm
MgA2 + 2H2O + Heat
= Mg(OH)2 + 2HA
T = 500 °C; P = 1 atm
Mg(OH)2 + CO2 = MgCO3
+ H2O
T = 300 °C; P = 20 bar
Products are separated

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P.K. Naraharisetti et al.
the process flow sheet.
The various steps in the iPEAD economic evaluation can be listed as
follows:
1. The experimental data is collected from researchers/literature. This
information includes types and quantities of raw materials and in-
termediates, reaction conditions & time, conversions and yields,
output composition and quantities, etc.
2. From the experimental data, a mass balance and energy balance is
performed and a flowsheet is designed that includes possible heat
integration.
3. From the flow sheet, the major equipment involved is identified and
sized according to a ‘Basis of Design’. The ‘Basis of Design’ is usually
between 100 k tonne/yr to 1 M tonnes/yr. For the purpose of this
work, we consider the ‘Basis of Design’ as 1 M tonne/yr mineral ore.
4. The costs of this major equipment (CapEx) are estimated based on
known data and engineering references which are incorporated in
the iPEAD tool. The operational costs (OpEx) are also estimated,
taking into account the utilities such as energy in various forms,
steam and raw materials that are required for process operations.
5. The production cost is calculated as a function of CapEx, OpEx and
the required Return on Investment (ROI).
The production cost is calculated from the CapEx and OpEx as fol-
lows:
Production Cost = 0.154 × CapEx + ROI × CapEx + OpEx (1)
where, the factor 0.154 is used to account for the fixed cost (de-
preciation of 10 yrs. if not stated, manpower costs, plant overheads,
maintenance, among others) of operating the production facility and
ROI is the return on investment that is expected. Typically, an ROI of
16% is considered. However, for the purpose of this work, ROI is not
considered as mineralization is expected to be a chemical process for
sustainability and societal good and not for profit.
It can be seen that the production cost can be estimated from the
CapEx and OpEx and it is important that these are estimates are reli-
able. OpEx is calculated as the combined cost of raw materials, inter-
mediates and energy/utilities. Hence, it is important that energy re-
quirements around various unit operations are performed and
preliminary heat integration is considered wherever possible.
In this work we obtain CapEx by multiplying Major Equipment Costs
by a Lang factor of 5. The basis for this is given in this section. CapEx is
calculated using the following Eqs. (Eq. 2–5). The methodology is based
on what is described by Peters & Timmerhaus [130].
CapEx = ISBL + OSBL (2)
where ISBL is Inside Battery Limits (Major Equipment and associated
infrastructure) and OSBL is Outside Battery Limits (tankage, roads etc).
Further, ISBL and OSBL are calculated as:
ISBL = Direct Costs + Indirect Costs (3a)
OSBL = 0.2 × ISBL (3b)
Therefore,
CapEx = 1.2 × (Direct Costs + Indirect Costs) (4a)
The details on calculation of ‘Direct Costs’ and ‘Indirect Costs’ are
given in Table 5 and Table 6. Hence, CapEx can be written as
CapEx = 1.2 × (2.9 × MEC + 0.5 × 2.9 × MEC) (4b)
CapEx = 5.22 MEC 5 MEC (5)
Hence, we multiply Major Equipment Costs with a factor of 5 to get
CapEx. Here, it must be emphasised that the value of 5 is a conservative
estimate and actual investment costs range between 3 and 10 times the
costs of Major Equipment.
The capital cost of the various equipment is taken from Aspen
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Renewable and Sustainable Energy Reviews 99 (2019) 220–233
Table 5
Various factors used in the calculation of ‘Direct Costs’.
Direct Costs As a factor of MEC
Major Equipment Costs (MEC) 1.00
Equipment erection 0.40
Piping 0.70
Instrumentation 0.20
Electrical 0.10
Buildings 0.15
Storages 0.15
Site development 0.05
Ancillary buildings 0.15
TOTAL DIRECT COST = 2.90 × MEC.
Table 6
Various factors used in the calculation of ‘Indirect Costs’.
Indirect costs As a factor of direct costs
Design and engineering 0.3
Contractor's fee 0.1
Contingency 0.1
TOTAL INDIRECT COSTS = 0.5 ×Direct Costs.
TOTAL INDIRECT COSTS = 4.35MEC.
Capital Cost Estimator 7.3.1 (ACCE) [131] which used data from 2010
and from other sources; further, the costs are normalized to current
CEPCI. This data is used to develop simple mathematical models and
these models are used in an MS Excel based software tool, iPEAD, where
we perform the flow sheeting; mass and energy balance calculations,
and estimate the OpEx and CapEx. We base our estimates on Carbon
Steel as the material of construction; however, more expensive steels
are used in reality. For equipment costing from Aspen, we use “Installed
Cost” from ACCE (which includes total material and manpower cost) as
our Major Equipment Cost (MEC). The “Installed Cost” in ACCE is 1.5–2
times the “Bare Module Cost”. In our calculation, we are neglecting the
material of construction, which can be a factor of 1 (carbon steel) to 15
(hastelloy). Thus, our calculation of CapEx as 5 × MEC by using “In-
stalled Cost” rather than “Bare Module Cost” is reasonable.
For the purpose of validation, we have used iPEAD to estimate the
Capital Expenses (CapEx) of six different processes that are available in
open literature. These are from technical reports by professional and
commercial agencies or plant owners and the comparison of CapEx
from literature vs. CapEx estimated using iPEAD is presented in Table 4
(extracted from [132]). The results show a difference of between -10%
& 25% between the CapEx estimated by iPEAD and the technical re-
ports, which is within the expected accuracy range in the early stage of
process development. This validates that iPEAD methodology is reliable
for preliminary economic analysis. In addition to the validation, we
have earlier performed economic evaluation of about twenty different
technologies that are being developed in ICES [132] and a couple of
process economic evaluations from amongst the twenty were presented
at AIChE Annual meeting, 2015 [133].
4.2. Process conditions and basis of design
Data for the DAC process is taken from the pioneering research work
that has been published earlier [3115]. Here, we perform process
evaluation of their process for five different scenarios where three
different minerals were used and the operating conditions optimized by
the researchers. This helps us understand the energy and cost drivers for
CO2 mineralization. Fig. 2 shows the schematic of the CO2 miner-
alization process. Briefly, the mineral undergoes grinding and the final
particle size is dependent on the type of mineral ore and the scenario
being studied. Further, Olivine and Wollastonite are directly used in
carbonation step upon grinding; however Serpentine undergoes
P.K. Naraharisetti et al. Renewable and Sustainable Energy Reviews 99 (2019) 220–233

Fig. 2. Schematic of the DAC process that is analysed in this work. Modified PFD based on process described in [10,140]. It is assumed that pure CO2 is available at
5 bar. In the case of Wollastonite, CO2 is directly compressed to reactor pressure (and remains in gas form) and additional heat is not necessary to heat the CO2.

Table 7
The Table shows the various minerals and the operating conditions, and mineralization capacity based on data in [10] for a 1 M tonnes/yr mineral processing plant.
Mineral flow 42.35 m3/h; Water for slurry 247.06 m3/h (30% w/v); Operating hrs/yr 8500 hrs; sp. gravity of mineral 2.5. Serpentine losses 10% weight as moisture
in calcination.
DAC 1 DAC 2 DAC 3 DAC 4 DAC 5

Olivine (Mg2SiO4) Serpentine (Mg3Si2O5(OH)4) Wollostonite (CaSiO3) Olivine (Mg2SiO4) Serpentine (Mg3Si2O5(OH)4)
Temperature (°C) 185 155 100 185 155
Pressure (atm) 150 115 40 150 115
Mineral Conversion 81% 92% 82% 61% 62%
Residence Time (hrs) 6 6 1 6 6
Particle size after grinding (µm) 10 38 10 38 75
CO2 capacity (tonnes/yr) 505,185 400,889 347,600 505,185 400,889
CO2 converted (tonnes/yr) 409,200 368,818 285,032 308,163 248,551

calcination in order to eliminate the hydrated water. Once the carbo-
nation process is complete, heat recovery is achieved via a heat ex-
changer; however it is assumed that water used for slurry preparation is
not recovered and any costs associated with use of water (30% w/v
slurry [3]) is negligible when compared to cost of carbonation. These
processes are labelled as DAC 1 to DAC 5 (D1 to D5) and presented in
Table 7. The operating conditions, conversions, residence time in the
reactor and particle size are given in Table 7. It must be mentioned here
that pre-treatment of Olivine and Wollastonite involves grinding
whereas Serpentine must also be heat treated to remove the bonded
water. However, Olivine and Wollastonite are more finely ground and
hence the total energy required for different types of ores must be
considered appropriately and the data for the same is taken from [7].
Two cases each are analysed for Olivine and Serpentine and one case for
Wollastonite is analysed. From data presented in [3] and reproduced in
Table 7, we can see that conversion is directly related to the particle
size. In view of this, it is important to understand the effect of enhan-
cing the conversion by using more energy for grinding.
The detailed CO2 penalty and energy penalty data are presented in
[7]; however, for the sake of completeness, the summary of the energy
demand for the mineralization processes is presented here. Figs. 3a & 3b
show the energy demand for the different process steps. Energy use is in
two forms, electricity (Fig. 3a) and heat (Fig. 3b). There is no heat in-
tegration possible when electricity is used; however heat integration
within the pre-treatment process and inside the reactor is possible. The
heat demand and possible heat integration is shown in Fig. 3b. It must
be mentioned here that the heat recovered in a given process step, pre-
treatment or reactor, can only be used in that particular step but not
elsewhere. Hence, any excess energy coming out of the reactor due to a
large exothermic energy is assumed to be waste. This assumption is
made especially since heat recovery from the products of the reactor,
which is in the form of slurry is usually done in spiral heat exchangers
and it is known that such heat exchanger have low efficiency and are
prone to clogging. While the conversions presented in Table 7 are be-
tween 61% and 92% in 6 h, other researchers have observed that it is
possible to achieve 70% conversion of Olivine in 4 hrs and 90% con-
version in less than 24 hrs at a temperature of 180 °C and 20 bar
pressure [129]. It must be noted here that the slurry concentration is
9% which is less than the 30% concentration that used in [3]. However,
these data [129] are not used in this work since low slurry concentra-
tions leads to large CapEx.
Table 7 shows the metal content of the different mineral ores. The
‘Basis of Design’ of this process is 1 M tonnes/yr of Mineral ore. From
the metal content, the maximum amount of CO2 that can be mineralized
and the amount of CO2 that can be mineralized at the experimental
conditions (given in Table 7) can be calculated and these are also shown
in Table 7. We note here that there is a 10% weight loss of Serpentine
mineral due to calcination.

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Table 8
A: CapEx of a 1 M tonnes/yr mineral processing plant. Units: M$/tonne.
DAC 1 DAC 2 DAC 3 DAC 4 DAC 5 Comments

High Pressure 287.4 200.6 30.2 358.9 168.8 1 M tonnes/yr

Reactor mineral
Compressor and 107.4 95.3 83.1 107.0 103.5 processing
Heat plant
Exchangers
for reactor
Pre-treatment 6.2 17.5 6.2 17.5 17.5
TOTAL 400.9 313.4 119.5 483.4 289.8
CapEx 979.8 849.7 419.4 1568.5 1165.8 1 M tonnes/yr
CO2 captured

subsequently the costs of the pressure reactor itself) in DAC5 is lower,

we identify a direct correlation between the pressure conditions re-
quirements for a process and it’s CapEx.
The overall production cost is highly affected by the operating costs
(OpEx) of the DAC processes; depreciation, conversion, purchased costs
of CO2 and the feedstock minerals are the main factors influencing the
OpEx. The impacts of these factors are studied in section below to de-
termine their effects on the overall cost structure.

4.3.1. Capital costs (per tonne mineral)

Fig. 3. A. Use of electricity by the different steps in the CO2 mineralization
process. Energy demand for cooling CO2 (after compression) is negligible but
not zero. B. Use of heat energy and possible heat recovery in the two main
process steps i.e., in Pre-treatment step and in Reactor. If net energy is negative
(excess of exothermic energy is available), it cannot be recovered and sold and
is thus assumed to be wasted.
4.3. Cost calculations
The process costs for DAC are found to be highly dependent on
CapEx, due to their requirements for high pressure equipment. The
largest cost factor in DAC processes is typically the pressure reactor.
This is evident when we consider the two cases DAC3 and DAC4. The
required pressure and temperature is relatively low (40 bar and 100 °C)
in DAC3, where Wollastonite is used as the feed material for carbona-
tion. As a result, the CapEx for DAC3 is much lower than the other 4
DAC processes considered in this work. However in DAC4, due to a
combination of low conversions and high pressures, the CapEx for the
high pressure reactor dominates the overall cost structure, resulting in
its CapEx being 4 times larger than the CapEx of DAC3.
Also, although the degree of reaction conversions are similar for
DAC 4 and DAC5, their CapEx are significantly different, with DAC5
being nearly 40% less expensive in terms of equipment investment. The
reason for this, again, lies with the costs associated with the high
pressure reactor. From the fact that pressure requirements (and
Table 8 shows the CapEx of the various Scenarios for a 1 M tonnes/
yr mineral processing plant. It must be noted here that the amount of
CO2 that can be captured in each scenario is different (depends on
mineral composition and metal type, Table 7). We can see that the
CapEx is the lowest when Wollastonite is used and this can be directly
attributed to the shorter residence time of 1 h. Briefly, when the re-
sidence time is the same, as in the case of Olivine and Serpentine, CapEx
for Serpentine is lower and this can be attributed to the lower operating
pressure. We can see that CapEx follows the order DAC3 < DAC
5 < DAC 2 < DAC 1 < DAC 4 when we do not include conversion.
We can use data from Table 7 (conversion) to calculate the CapEx
per tonne of CO2 captured and this is equal to $980, $850, $419, $1569
and $1166 respectively for each of the five processes. We can clearly see
the difference between the CapEx per tonne of mineral and CapEx per
tonne of CO2 captured and this is obviously due to the type of mineral
and the conversion that is achieved at the given operating conditions.
The CapEx follows the order DAC3 < DAC 2 < DAC 1 < DAC
5 < DAC 4 when we include the conversion. It can be seen clearly that
conversion has a great role in determining the CapEx/tonne of CO2
captured. DAC3 is clearly the cheapest and DAC4 is clearly the costliest
both the times.
When conversion is low, more of the mineral is required in the re-
actors and this increases the CapEx per tonne of CO2 captured. The
capital expenses form the initial cost outlay to build and commission
the plant and these details are presented in Table 8 on per tonne mi-
neral basis. Briefly, they are between $120 (DAC3) and $483 (DAC4)
per tonne mineral processed.
4.3.2. Production cost
Table 9 shows the production cost of the CO2 mineralization pro-
cess. It stands between $238 & $393 where the lowest cost is when
Wollastonite is used. We can see that the OpEx is almost the same ir-
respective of the particle size or conversion, but the production cost is
different due to the fixed cost associated with running a large plant that
has poor conversion.
It is thus clear from the earlier discussion that both CO2 penalty and
CapEx are directly related to the particle size and conversion. Hence, in
order to develop an economical process it is important that the oper-
ating conditions are selected carefully. At $238 per tonne of CO2 cap-
tured ($70 per tonne of pure CO2 and $168 as other costs), the process
is not economically viable unless there is a mechanism to take carbon

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Table 9 millions of square kilometres, much larger than the amount of carbo-
Production Cost – Basis: $/tonne CO2 captured unless otherwise stated. nates that can ever be produced and it has an added advantage in that it
PC=OpEx + 0.154 *CapEx (Eq. 3b). Cost of Mineral: $10/tonne. Cost of pure can grow bushes and shrubs that capture carbon dioxide. If there is
CO2 at 70$/tonne. Amount and Cost of Heat and Electricity are taken from [7]. scope for mixing the CO2 mineralization products with compost (say in
Type of fuel is not considered when using the cost of heat/electricity. CP: Total
a conservative ratio of 3:1), then about 10 G tonnes/yr of compost must
CO2 Penalty (Fig. 4a; for natural gas only. CP for the case of coal is not used in
be produced. Since biomass is the primary raw material for compost
this table).
production, it is unlikely that soil-remediation would serve as a primary
DAC 1 DAC 2 DAC 3 DAC 4 DAC 5 market for CO2 mineralization products. In view of this, we must
carefully analyse alternative markets that can generate income to cover
Cost of pure CO2 70.0 70.0 70.0 70.0 70.0
Cost of Mineral 24.4 27.1 35.1 32.5 40.2 the costs of the CO2 mineralization process.
Cost of Heat 0.0 4.3 0.0 2.8 7.3 We have earlier analysed the size of the market and the potential
Cost of Elec. 75.0 39.7 68.6 45.9 23.6 market for the mineralization products. It was observed that low value
Total OpEx OpEx 169.4 141.2 173.7 151.2 141.1 uses such as landfill and construction material are possible uses for
OpEx per tonne of CO2 OpEx/(1- 245.0 176.2 253.1 191.9 172.0
avoided CP)
products of direct CO2 mineralization. We assume that the price of the
Production Cost (per PC 320.3 272.0 238.3 392.8 320.6 product for low value applications is usually between 10 and 30
tonne of CO2 $/tonne of material which is the same as the price of construction sand
captured) in Singapore. Since 2.75–4 tonnes of ore/ton of CO2 is required, the
Production Cost (per PC/(1- 465.4 343.3 346.0 503.6 396.1
total product weight is between 3.75 and 5 tonnes/tonne of CO2 mi-
tonne of CO2 CP)
avoided) neralized. This translates to an income of about 37.5–150 $/tonne of
CO2 mineralized. In comparison, the lowest value we have observed for
DAC5 is $202/tonne of CO2 captured and much of the production cost
credits or external financing is necessary. This may draw us to a qua- is due to CapEx. In view of this, the CO2 mineralization process must be
litative conclusion that we must select mild operating conditions and developed such that the production cost is as low as possible and this
target higher conversion with larger particles. can only be possible if the CapEx is low. In other words, subsidy from
In conclusion, it is important to note that the cost of the CO2 mi- governments for the construction of CO2 capture may be necessary,
neralization process is not high, while it is not very low either. In view while operating costs can be recovered by selling the products.
of this it is necessary to do a scenario analysis on the possible ways in
which costs can be reduced. Further, it is worthwhile to explore the 4.5. Comparison with literature
possible revenue from sale of products from the CO2 mineralization
process. However, cost per tonne of CO2 captured is not the same as In this work, we have performed a detailed evaluation of the DAC
cost per tonne of CO2 avoided. This is because each process consumes process. For better comparison it is apt to compare our cost estimates
different forms and amounts of energy and there are CO2 emissions with those that were presented by [3] along with other economic
associated with use of this energy. Hence, a different measure called the evaluations that are presented in literature. IPCC [135] has reported
cost of CO2 avoided must be calculated to get a complete under- values of between $55 and $430 per tonne of CO2 captured and these
standing. To make this discussion complete, it is important to discuss estimates were based on the calculations performed by [3]. Further, [3]
the cost per tonne of CO2 avoided. For the benefit of the readers, CO2 has reported that the cost is between $78 and $538 per tonne of CO2
and Energy Penalty from [7] are reproduced here (Figs. 4a & 4b) and avoided. It must be mentioned here that the costs presented by [3] and
this data can be used to calculate the cost of CO2 avoided. The cost per IPCC do not include capital costs. More recently, Hitch & Dipple [136]
tonne of CO2 avoided for both the OpEx and Production Cost, when estimated that the operating cost of CO2 capture is between $28 and
natural gas is used as fuel is presented in Table 9. $238 and the most likely cost is $83; they have reported a CO2 avoid-
ance factor of 0.77. In addition they have reported that the capital cost
of a CO2 capture plant that captures 2 M tonnes/yr is $139 Million. This
4.4. Market size of the products is equivalent to 90 $/tonne of CO2 avoided (~139/2/0.77). In com-
parison, we estimate that the cost of CO2 mineralization ranges between
As we present the details of the economic analysis it is important to $343 and $504 per tonne avoided if CapEx is included and between
understand the size of the market for the products. Details of both high $172 and $253 if only the OpEx is considered when natural gas is used
value and low value use of the products are presented elsewhere [134]. as fuel. Overall, we can conclude that the range of values reported in
Briefly, they can be classified as carbonates, silica and iron oxide. It is literature [3,135,136] and this work, all are close to each other when
obvious that the market for high value applications of carbonates (fil- CapEx is not included.
lers, fire-retardants etc.), silica (semi-conductors, ceramics etc.) and We have observed earlier that the income from CO2 mineralization
iron-oxide (pigments, paints etc.) is rather limited and hence we must process is about 37.5–150 $/tonne of CO2 captured. In comparison, the
focus on low to medium value applications. These include use of car- OpEx of the CO2 mineralization processes was observed to between
bonates for land reclamation, filler in construction industry, and for soil $172 and $253 per tonne of CO2 avoided (Table 9) and this includes the
remediation and the use of iron oxide in the iron and steel industry. cost of pure CO2 at 70$/tonne and ore at 10$/tonne. We can see that
To elaborate on the potential for the use of carbonates as for land the majority of the operational costs are due to the cost of ore and pure
reclamation, consider the shallow waters that are about 50 m deep. CO2 and the operational costs associated with the CO2 mineralization
About 125 M tonnes of carbonate is required to reclaim an area of 1 sq. process (heat and electricity) is rather less at $31 to $75 per tonne of
km area (assuming carbonate density is 2.5) and hence, about 250 sq. CO2 captured (Table 9). It is interesting to note here that although the
km/yr can be reclaimed every year if 9 Gt of CO2 is mineralized. fine grinding increases the overall conversion and reduces the CapEx,
Considering the size of the world’s largest cities, this land area is rather the OpEx per tonne of CO2 captured is more than that of DAC1 and this
small and hence, the effect on ocean environment due to land re- is primarily due to grinding. Hence, it may not always be appropriate to
clamation may be assumed to be small. Another end use which po- target high conversion via grinding.
tentially has large demand but has seen less focus could be the use of In addition to this, we have performed a scenario analysis con-
mineral carbonates for soil-remediation and/or conversion of deserts sidering a longer depreciation time of up to 40 yrs. and the availability
into semi-arid regions that may promote partial reforestation. The po- of ore at a lower cost of $5/tonne. For the purpose of the scenario
tential of land conversion to semi-arid zones is potentially in the analysis, we have considered DAC5 process as it reflects the most likely

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P.K. Naraharisetti et al.
Fig. 5. The figure shows the production cost per tonne of CO2 avoided as a
function of cost of pure CO2 and depreciation of the plant based on DAC5
process.
process conditions and conversion when the process is scaled-up. The
results of the scenario analysis have been presented in Fig. 5. It can be
seen (Fig. 5) that the cost can be as low as $170/tonne of CO2 avoided if
government policies allow longer depreciation times of 40 yrs. and
supply ore at a low cost.
4.6. Future directions
It must be emphasised here that the capital expenses must be dis-
cussed separately and they form the initial cost outlay to build and
commission the plant; these details are presented in Table 8 on per
tonne mineral, per tonne CO2 captured and per tonne CO2 avoided.
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Renewable and Sustainable Energy Reviews 99 (2019) 220–233
Fig. 4. A. The figure shows the CO2 penalty for the dif-
ferent processes [7] when Natural gas is the fuel. CO2
emissions (natural gas): 0.43 kg/kWh; 50.643 kg/GJ. Total
CO2 penalty is DAC1: 31.5%; DAC2: 21.7; DAC3: 30.5%;
DAC4: 22.5%; DAC5: 19.9%. Electricity penalty on power
plant is DAC1: 31.5%; DAC2: 16.1%; DAC3: 30.5%; DAC4:
19.0%; DAC5: 9.1%. B. The figure shows the CO2 penalty
for the different processes [7] when Coal is the fuel. CO2
emissions (coal): 0.996 kg/kWh; 89.92 kg/GJ. Total CO2
penalty is DAC1: 73.0%; DAC2: 47.3; DAC3: 70.6%; DAC4:
50.2%; DAC5: 40.2%. Electricity penalty on power plant is
DAC1: 73.0%; DAC2: 37.3%; DAC3: 70.6%; DAC4: 44.1%;
DAC5: 21.2%.
Since the net CO2 capture efficiency of natural gas based processes
(68–80%) is higher than that of the coal based processes (data not
presented here), we can expect a monumentally high amount of capital
investments for coal based CO2 mineralization processes when CO2
avoided is considered. We have calculated that the initial investment
outlay for CO2 mineralization process as being between $419 and
$1569 per tonne of CO2 captured. This translates to between $1003 and
$1774 per tonne of CO2 avoided when energy comes from natural gas.
This large investment outlay transforms itself into a large production
cost especially since production cost includes fixed costs associated
with the operation of a plant.
In view of this, we can conclude that DAC process is a potentially
economical process only if there is some form of government subsidy
for CapEx. Notwithstanding the subsidies, research must be focussed on
reducing the electricity penalty of the process and the cost of the pro-
cess must be reduced by reducing the cost of producing pure CO2 and
mineral ore. In view of this, we identify the following research areas:
1. Increase the CO2 capture efficiency and reduce the electricity pen-
alty by reducing the total energy required by the process. This can
also be achieved by optimizing conversion with the particle size and
the energy required for grinding and milling as parameters. Such a
study helps reduce the capital cost per tonne of CO2 captured to a
large extent and partially reduces the operational costs. Use of
chemical pre-treatments and/or use of buffers must also be explored
so that conversion of large particle mineral ores is increased.
2. The component of CO2 penalty which is related to the use of elec-
tricity (from natural gas or coal) can be reduced by using electricity
from solar/wind farms. In spite of this, the costs must be borne by
the society/governments and allocation of some amount of carbon
tax to mineralization processes may be one way to fund the capital/
operational costs.
P.K. Naraharisetti et al.
3. Reduce the cost of pure CO2 and mineral ore. This helps reduce the
operational costs.
4. Increase the depreciation time from 10 yrs. to may be 40 yrs.
In view of the above, it may be worthwhile to explore other pro-
cesses that use flue gas directly without any purification in order to
reduce the cost of CO2. Further, it would be of economic importance to
develop processes that produce valuable materials as products of the
CO2 mineralization process so that operational and capital expenses can
be offset by the income from these products [130–132]. These products
include magnesium/calcium carbonate, iron oxide and silica. The de-
mand for silica is of the order of millions of tonnes [137], that of car-
bonates is of the order of tens of millions of tonnes [134,138], while
that of iron oxide (to replace iron ore) is in the hundreds of millions of
tonnes [139]. In view of this, it may be worthwhile to develop processes
that have the two-fold advantages in the form using flue gas directly
and also generating income from products. Therefore, it may be im-
portant to develop integrated processes that consist of a main DAC
process that captures large amounts of CO2 from industrial sources, and
a smaller mineral upgrading process (for example a pH-swing aqueous
mineralization process) that can work with similar feed material and
produce high value-added products for sale to recover some of the costs
[26–28]. This arrangement can benefit both processes involved, as the
DAC process can help to bring down the overall CO2 penalty of the
integrated process, and the pH-swing process can bring in revenue to
reduce the overall costs of CCU.
5. Conclusions
In this work, we have performed the economic evaluation of the
DAC process which is a pioneer process that is implemented at pilot
scale. We conclude that Wollastonite is the mineral of choice for per-
forming CO2 mineralization at low cost. For the different minerals and
the scenarios that were analysed, the OpEx currently stands between
$172 & $245 per tonne of CO2 avoided when natural gas is used and the
production cost is between $343 and $504. Further, we have identified
that a minimum of three types of inputs are required for the CO2 mi-
neralization process in order to improve the kinetics of the rock
weathering process which occurs in Nature and that the type of mineral
ore influences the economics greatly. In view of this, it is important to
focus our research on selection of mineral ore, minimizing the elec-
tricity required by reducing the operating pressure, and on minimizing
the heat required by the process.
Acknowledgements
Financial support for this work under ICES/09-434A01 & ICES/12-
134A01 is gratefully acknowledged. We would like to thank Prof. Paul
Sharratt for his valuable advice. The support of colleagues in checking
some of the calculations is also acknowledged.
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