Journal of CO2 Utilization 60 (2022) 102000

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Journal of CO2 Utilization

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

Review article

An overview of utilizing CO2 for accelerated carbonation treatment in the

concrete industry
Liang Li , Min Wu *
Department of Civil and Architectural Engineering, Aarhus University, Aarhus C, 8000, Denmark

A R T I C L E I N F O A B S T R A C T

Keywords: Accelerated carbonation treatment as an effective approach of reducing the carbon footprint in the concrete
Accelerated carbonation industry is being investigated extensively. Such carbonation treatment converts gaseous CO2 into carbonate
CO2 sequestration minerals (or mineral CO2 sequestration). The present review provided a state-of-the-art summary on the relevant
Recycled concrete aggregate
carbonation strategies that have been investigated, with a special focus on identifying the remaining industrial
Fly ash
challenges and critical research gaps that need further investigation. Key parameters affecting pre-carbonation
Slag
treatments of recycled concrete aggregates, fly ash, and slag were examined systematically, including chemi­
cal compositions and particle sizes of the materials, temperature, pressure, and CO2 concentration. The CO2
uptake capacity and efficiency of the materials were compared with each other, and the environmental impact of
pre-carbonation treatment of fly ash and slag was approximated. After carbonation treatment, the incorporation
of those carbonated materials in cement-based composites was assessed. It was found that the rising CO2 uptake
of ingredient materials subjected to pre-carbonation treatment does not necessarily benefit the mechanical
properties of the cement-based composites with the carbonated materials. For a specific material, there may exist
a CO2 uptake threshold over which high CO2 uptake tends to be deleterious, e.g. for the mechanical properties. In
terms of the influence of accelerated carbonation curing on the compressive strength of cement-based composites
at early ages, both positive and negative influences were identified. Corresponding mechanisms behind such
contrary influences were critically discussed. It was noted that over-intensified early-age carbonation curing
could compromise the strength properties of cement-based composites both in the short and long terms.

1. Introduction
Nowadays, over 8.0% of total global carbon dioxide (CO2) emissions
are related to cement and concrete productions [1,2]. According to the
World Cement and Concrete Product Market Outlook 2020–2030, the
global cement and concrete product market was $370.1 billion in 2019
and is expected to grow at a compound annual growth rate of 12% from
2021. The global production of cement in 2030 is estimated to reach 5
billion tons worldwide [1]. The CO2 emissions from cement and con­
crete productions are likely to represent more than 10.0% of the total
global CO2 emissions in 2030–2050 [1]. With increasing pressure to
meet the worldwide high demand on cement-based materials yet to
reduce global greenhouse gas emissions, systematic strategies are crucial
for the sustainable development of the concrete industry [1,2]. One of
the current strategies is to achieve substitution of cement clinker by
supplementary cementitious materials [3–7], since the CO2 emission
from the production of cement clinker accounts for approximately 85%
of the total CO2 emission of concrete [8]. However, such a substitution
approach alone has been far from enough to meet the global CO2 miti­
gation target.
In [6,9–12], other strategies for lowering CO2 emissions and
improving concrete production have been put forward, including cap­
ture and utilization of flue gas from cement plants, development of
energy-efficient technologies for cement production, reuse and recycling
of industrial waste materials, and exploration on cement-free construc­
tion. Particularly, mineral CO2 sequestration as a relatively new CO2
mitigation option has developed rapidly in the past few decades and
presented encouraging environmental benefits [3,6,13–18]. In the
concrete industry, mineral CO2 sequestration can be understood as a
carbon capture and storage process that mainly involves the reaction of
CO2 with calcium bearing materials and the formation of calcium car­
bonates [19–22], as given by Eqs. (1) to (4):
Ca(OH)2 + CO2 → CaCO3 + H2O (1)

* Corresponding author.
E-mail address: mnwu@cae.au.dk (M. Wu).

https://doi.org/10.1016/j.jcou.2022.102000
Received 12 November 2021; Received in revised form 5 March 2022; Accepted 2 April 2022
Available online 9 April 2022
2212-9820/© 2022 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

C-S-H + CO2 → CaCO3 + SiO2 + nH2O (2) current knowledge gaps in the conduct of early-age carbonation curing
highlighted. Discussion and conclusions presented in this review are
C3S + (3-x)CO2 + yH2O → CxSHy + (3-x)CaCO3 (3) expected to offer valuable insights on the utilization of accelerated
carbonation treatment in the concrete industry and facilitate the
C2S + (2-x)CO2 + yH2O → CxSHy + (2-x)CaCO3 (4) decision-making process in the development of mineral CO2 sequestra­
tion technology.
Generally, the natural mineral CO2 sequestration of cement-based
composites during the service life is quite limited, due to the slow
2. CO2 sequestration by accelerated carbonation treatment
chemical kinetics of carbonation reactions [23–27]. To boost the CO2
sequestration capacity and efficiency, accelerated carbonation treat­
2.1. Mechanisms of mineral CO2 sequestration
ment has enjoyed important development recently [21,28–32]. The best
uses of accelerated carbonation treatment in the concrete industry
Generally, mineral sequestration of CO2 by industrial waste mate­
mainly focus on (i) pre-carbonation of industrial waste materials before
rials involves three crucial steps (as illustrated by Fig. 2): (A) leaching of
concrete mixing and (ii) early-age carbonation curing of cement-based
mineral (mainly, Ca2+) ions from solid to liquid; (B) dissolution of CO2
composites after mixing, as shown in Fig. 1. The industrial waste ma­
and formation of carbonate ions; and (C) carbonation reactions and
terials that are mostly investigated for mineral CO2 sequestration in the
formation of calcite particles and layers. In fact, these three steps are
concrete industry include fly ash, slag, recycled concrete aggregates
also three key processes determining the carbonation efficiency and
(RCA), etc. [9,33–35]. Fly ash and slag are byproducts of coal burning
capacity of the materials. It must be noted that liquid (or moisture) is
and metal manufacturing, and RCA are waste aggregates recycled from
always a necessary constituent in Steps A and B [46]. For the leaching of
demolished concrete. These waste materials all contain a certain amount
calcium ions in Step A, it is significantly affected by the total calcium
of calcium-bearing phases which enable CO2 sequestration to form
content, particle sizes, and microstructures of the raw mineral materials
carbonate compounds. Early-age carbonation treatment is a means of
[47,48]. Besides, increasing temperature can also enhance calcium
curing fresh concrete via accelerated carbonation, which has gained
leaching. However, the growth of the calcite layer (see Fig. 2) caused by
increasing attention recently. Compared to accelerated carbonation
the precipitation of calcite particles is somehow behaves as a barrier for
treatment of industrial waste materials, the early-age carbonation curing
the further leaching of calcium [48]. In the process of mineral seques­
of cement-based composites is a more complex process. On one hand,
tration of CO2, the formation of carbonate ions in liquid is affected, e.g.
cement-based composites with different constitutes tend to have varied
by CO2 concentration, temperature, and pressure [49], whereas kinetics
chemical compositions and microporous structures, which complicates
of carbonation reactions is primarily temperature-dependent.
carbonation conditions [19–21,23,36–38]. On the other hand, carbon­
ation and hydration reactions of cement-based materials take place
2.2. Main methodology
simultaneously at early ages, and there exists a coupling effect between
the two reactions [37,39]. Nowadays, it has been widely acknowledged
So far, industrial-scale studies and applications of carbonation
that early-age carbonation curing can significantly influence the per­
techniques in the concrete industry are rather limited, and consequently,
formance of cement-based composites at early ages as well as at late ages
the current focus is primarily placed on laboratory-scale studies. In the
[36–38,40–44]. In practice, accelerated early-age carbonation treatment
laboratory, a wide range of accelerated carbonation approaches has
holds enormous potential for curing precast concrete elements which
been proposed and utilized. Compared with natural carbonation,
accounts for around 10% of world concrete consumed per year [10,20,
accelerated carbonation treatment can increase both the carbonation
45].
speed and the carbon storage capacity of materials. According to expo­
In this paper, the accelerated carbonations of fly ash, slag, and RCA
sure conditions of the materials in the mineralization process of CO2,
were reviewed systematically. On that basis, a special emphasis was laid
typical carbonation treatments can be roughly categorized into two
in analyzing the characteristics of cement-based composites containing
main types [50–52]: Gas-solid Carbonation (or dry carbonation) and
the carbonated materials as substitutes for aggregates or cementitious
Aqueous Carbonation (or fluid-solid carbonation). At present, acceler­
materials. After that, the complicated influence of early-age carbonation
ated carbonation treatment using supercritical CO2 has also been re­
curing on the properties of cement-based composites was explored, with
ported [21,53], but it is out of the scope of this review. Briefly, gas-solid
carbonation is a gaseous CO2 mineral sequestration process carried out
under a given relative humidity (RH) condition [52,54–57], as shown in
Fig. 3(a). By contrast, the typical feature of aqueous carbonation is that
solid mineral waste is immersed in a liquid mixture in which gaseous
CO2 is injected in [50,58–61], as illustrated in Fig. 3(b). In both gas-solid
and aqueous carbonation processes, the pressure and temperature of the
reactions are generally adjustable, as well as CO2 concentration and flow
rate.

Fig. 1. Two mineral CO2 sequestration strategies highlighted in the pre­

sent paper. Fig. 2. Schematic diagram of mineral CO2 sequestration.

2
L. Li and M. Wu
Fig. 3. Simplified diagrams of (a) gas-solid carbonation and (b) aqueous
carbonation.
2.3. Determinations of carbonation capacity and efficiency
In the concrete industry, the main purposes of performing acceler­
ated carbonation treatment are (i) reducing the carbon footprint and (ii)
improving the performance of construction materials. The two objec­
tives are both closely related to a crucial parameter – the CO2 uptake
capacity of the materials. Briefly, the CO2 uptake capacity (or namely,
CO2 sequestration capacity) can be deemed as the net uptake of CO2 as a
mass percentage of the original material before carbonation [62–64], as
given by Eq. (5). Generally, the determination of the CO2 uptake ca­
pacity can be measured by different methods, such as the mass gain
method, the mass curve method, and the thermogravimetric analysis
[19,20,65–67].
CO2− = MCO2 /Mc × 100 (5)
uptake
where, MCO2 is the mass of CO2 that has been successfully sequestered in
carbonation treatment and Mc is the original mass of the material before
carbonation treatment.
Besides the CO2 sequestration capacity, the other key parameter to
quantify the carbonation effect of materials is the carbonation efficiency
(or degree of carbonation) [58,68–70], as given by Eq. (6). It can be
referred to as the successfully captured mass of CO2 (MCO2 ) by a material
under a given condition compared to the theoretical CO2 sequestration
potential (Mth ) determined based on Steinour’s formula [71] or Hunt­
zinger’s formula [70]. For a given material, the higher the carbonation
capacity, the higher the carbonation efficiency. For different materials
exposed to varied carbonation conditions, the higher the carbonation
efficiency, the better the mineral CO2 sequestration effect.
CO2− eff = MCO2 /Mth × 100 (6)
3. Accelerated carbonation of industrial waste materials
First of all, a detailed literature review on the pre-carbonation
treatment of RCA, fly ash, slag, and other industrial waste materials
was performed. The main purpose aimed to summarize favorable
accelerated carbonation conditions proposed in the literature and
identify key factors influencing the carbonation effect of the materials.
Also, gas-solid carbonation and aqueous carbonation both were included
and analyzed comprehensively, as given below.
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Journal of CO2 Utilization 60 (2022) 102000
3.1. RCA
To achieve sustainable development of the concrete industry, the
recycling and reuse of crushed old concrete as partial replacement of
natural aggregate in new concrete mixtures have been widely investi­
gated [72–77]. However, most studies present that the incorporation of
RCA tends to degrade the mechanical properties of concrete [72,78–80],
due mainly to the high water absorption capacity and porosity of RCA.
To promote the recycling and reuse of RCA, pre-carbonation treatment
(or carbon-conditioning) had been suggested [35,50,61,81–85]. How­
ever, although the carbon-conditioning benefits the performance
enhancement of RCA, it also consumes energy. To achieve cost-effective
carbonation treatment of RCA, a wide variety of carbonation tests had
been carried out, as listed in Table 1. It can be observed that aqueous
carbonation of RCA can achieve remarkably higher CO2 uptake within
10 min than the gas-solid carbonation over several days. This mainly
results from (a) submerging RCA in liquid speeds up the leaching of
mineral (mainly Ca2+) ions, and (b) dissolution of CO2 and formation of
carbonate ions are accelerated in aqueous carbonation. Despite a better
carbonation effect at a laboratory scale, aqueous carbonation has not
been suggested to conduct the industrial-level production of carbonated
RCA due to its complexity and high energy consumption. By contrast,
the gas-solid carbonation of RCA seems to be more applicable in prac­
tice. Accordingly, this section pays more attention to those factors
affecting the carbon-conditioning of RCA under dry carbonation con­
ditions. Concerning the utilization of aqueous carbonation, an in-depth
discussion is presented in the following sections.
From Table 1, it can be recognized that particle size affects the
carbon-conditioning of RCA significantly. In general, RCA with small
particle sizes appears to have a high CO2 sequestration capacity [56,81].
This is attributed to (i) small RCA tend to have a high mass percentage of
old mortars containing high calcium composition available for carbon­
ation [54,79,86] and (ii) small RCA have a larger specific surface area
(in contact with CO2) compared to RCA with large particles [91]. In [54,
92], it was proposed that with the decrease in the diameter of RCA
particles, an exponential increase in the CO2 uptake capacity would
occur. In addition, the moisture content (or RH) of RCA plays an
important role in carbonation. Because carbonation reactions hardly
take place at low moisture content, most previous studies suggested an
optimal RH ranging between 50% and 70% for gas-solid carbonation at
ambient temperature [19,86,93,94]. It is believed that too high moisture
content prevents CO2 from penetrating into the inner part of samples
[31,87,91,94,95], therefore compromising CO2 diffusion and overall
carbonation effect. However, for the carbonation at elevated tempera­
ture, high water content may benefit carbonation [91]. This is because
rising temperature accelerates the diffusion of CO2 and the leaching of
calcium ions [48,91] yet reduces the solubility of CO2 and calcium ions
in liquid. To compensate the reduced solubility at elevated temperature,
a high-water content is therefore needed.
In addition, the concentration of CO2 used for performing carbon­
ation treatment can also affect the carbon-conditioning of RCA. In [96],
it was found that rising CO2 concentration from atmospheric level
(around 0.03%) to around 20–40% considerably accelerated the
carbonation of RCA. However, the continuous rising of CO2 concentra­
tion from 40% to 100% would only marginally affect the carbonation
effect. In [97], a consistent conclusion was obtained claiming that rising
CO2 concentration would not continuously enhance carbonation of
cement paste. Similar to the impact of CO2 concentration, it was also
noted that increasing CO2 partial pressure from 0.003 to 0.01 MPa
considerably accelerated carbonation of mortars, whereas the increase
of CO2 partial pressure from 0.01 to 0.05 MPa had negligible influence
[98]. In [99], a similar conclusion was put forward that the increase in
pressure from 0.07 to 0.41 MPa had no significant effect on the accel­
erated carbonation of concrete samples. Therefore, for dry carbonation
of cement-based composites, a slight positive pressure of CO2 seems to
be desirable [31,54]. In [54], 0.01 MPa was suggested for the
L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Table 1 Table 1 (continued )

Carbon-conditioning of RCA subjected to varied conditions. Ref. Carbonation Features of RCA Duration Carbonation
Ref. Carbonation Features of RCA Duration Carbonation conditions capacity
conditions capacity ○Ambient 3.78-9.65 %
[54] Gas-solid ●Particle size 24 h 3.8 % temperature ●Mean particle size
○Atmospheric of 0.037 mm
carbonation: between 5.0-10.0
○Temperature of 25 mm pressure
o ○CO concentration
C 2
○RH of 50 ± 5% of 18.2 %
○CO concentration
2
of 99.5 %
○Pressure of 10 kPa carbonation of RCA at a commercial scale. In essence, pressure and CO2
[56] Gas-solid ●Particle size 28 - 91 d 1.1 % concentration impact dry carbonation based mainly on their influences
carbonation: between 0.5-5.0
○Temperature of 20
on the diffusion of CO2 and formation of carbonate ions in pore liquid
mm
o
C (see Fig. 2). High CO2 concentration can accelerate the formation of
○RH of 65 % carbonate ions in liquid but hardly affect the solubility of CO2, which is
○Atmospheric CO
2 dependent mainly on temperature and pressure. In general, temperature
concentration rise would compromise the increased dissolution of CO2 in water
○Atmospheric

pressure
induced by rising pressure [100], as shown in Fig. 4.
[81] Gas-solid ●Particle size 7d 1.8 % In fact, the carbonation of RAC is essentially the carbonation of
carbonation: between 0.16-2.5 hardened cement paste attached to the surface. In [91,101], the tem­
○Temperature of 20 mm perature dependency of accelerated dry carbonation of hardened
± 2 oC
○RH of 60 ± 5%
cement paste was explored. The measured experimental results in [91]
○CO concentration
2
showed that the highest CO2 sequestration appeared at approximately
of 20 ± 2 % 80 ◦ C, while a much higher temperature over 80 ◦ C (up to 300 ◦ C)
[82] Gas-solid ●Particle size 24 h 0.9 % reduced the final CO2 uptake. A similar finding was reported in [101] in
carbonation: between 12.5-19.0 which the CO2 uptake studied in a temperature range between 20 and 80
○Temperature of 21 mm
± 1 oC
◦
C reached the maximum at around 50 ◦ C. Theoretically, rising tem­
○RH of 50 ± 1% perature contributes to the accelerated leaching of calcium ions and fast
○Pressure between kinetics of carbonation reactions, indicating high CO2 uptake capacity
241-276 kPa and speed. However, the rising temperature also promotes the formation
○CO concentration
2
of calcite layer and calcite particles. As shown in Fig. 5, the calcite layer
99.9 %
[86] Gas-solid ●Particle size 24 h 0.49-0.81 % attached to the surface of minerals can delay the leaching of calcium
carbonation: between 5.0-20.0 ions, and the calcite particles can densify porous structures of cement
○Temperature of 25 mm paste and thereby hinder the diffusion and dissolution of CO2 [102]. As a
± 3 oC result, rising temperature imposes two mutually opposing effects on the
○Pressure of 10 and

500 kPa
carbonation process of materials. Due to the complexity of the influence
○CO concentration
2
of temperature on mineral CO2 sequestration, further explanation is
of 100 % given in the following sections.
[87] Gas-solid ●Particle size 24 h 5.0 %
carbonation: between 1.0-4.0
○Temperatures of 20 mm
and 40 oC ●Porosity of 13.8
○Atmospheric %
pressure
○CO concentration
2
between 15-100 %
[50] Aqueous ●Particle size 10 min 10.7 %
carbonation: between 0.15-5.0
○Atmospheric mm
pressure
○CO concentration
2
of 98 %
[88] Aqueous ●Particle size 10 min 11.6 %
carbonation: between 5.0-10.0
○Temperature of 25 mm
o
C
○Atmospheric

pressure
○CO concentration
2
of 99.9 %
[89] Aqueous ●Mass percentage 10 min 5.7 %
carbonation: of CaO of 30.84 %
○Ambient ●Particle size
temperature below 0.5 mm
○Pressure of 0.99

MPa
○CO concentration
2
of 18.2 %
[90] Aqueous ●Mass percentage 15 min 2.3 %
carbonation: of CaO between
Fig. 4. Solubility of CO2 in water affected by temperature and pressure, data
from [100].

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L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Table 2
Reported carbonation capacity and efficiency of fly ash in previous studies.
Ref. Carbonation Carbonation Carbonation Remarks
approach capacity efficiency

[58] Aqueous 2.6 % 82 % ●Low-calcium fly ash

(5 % CaO, by mass)
●Mean particle size
of 40 µm
●Temperature of 30
o
C
[59] Aqueous 0.8 % - ●Low-calcium fly ash
(7.0 % CaO)
●Ambient
temperature and
pressure conditions
Fig. 5. An illustration of the influence of carbonation products on carbonation
[60] Aqueous 2.7 % 13.9 % ●High-calcium fly
process (note: the calcite layer can delay the leaching of calcium ions, and the
ash (24.8 % CaO)
calcite particles can hinder the diffusion and dissolution of CO2). with maximum
particle sizes of 1.18
3.2. Fly ash mm
●Pressure of
approximately 3.0
A wide variety of laboratory-scale studies had been carried out to MPa
explore the potential of using fly ash as a material for mineral CO2 [68] Aqueous 3.2 % 83.5 % ●Low-calcium fly ash
sequestration, as summarized in Table 2. It can be noted that the (3.35 % CaO)
measured CO2 uptake of different fly ashes significantly varied within a ●Carbonation
temperature of 30 oC
wide range between 0.77% and 26.4%. To identify possible reasons [69] Aqueous 21.0 % 84 % ●High-calcium fly
responsible for such considerable variation of the CO2 uptake, key fac­ ash
tors affecting carbonation treatment of fly ash were analyzed in this ●High temperature
section, including but not limited to chemical compositions, particles of 90 oC
[103] Aqueous 0.77 % - ●High-calcium fly
sizes, temperature, CO2 concentration, pressure, etc. For the extremely
ash
low CO2 sequestration capacity (0.77%) measured in [103], the main ●Mean particle size
reason is that before the determination of the carbonation capacity of of 0.9 mm
the fly ash, long-term natural carbonation had taken place. Disregarding ●Long-term
atmospheric
such measurement error, it can be observed that fly ashes with high
carbonation taking
calcium content basically present a high carbonation capacity. However, place before the
it should be underlined that due to the constant solubility of Ca-bearing accelerated aqueous
minerals (especially Ca(OH)2) in water under a given condition (for carbonation of fly ash
example, a fixed liquid-to-solid ratio in aqueous carbonation) [59], too [104] Aqueous 13.2 % 24 % ●Fly ash with high
Ca/Mg-bearing
high calcium content of fly ash may not lead to the increased carbon­
minerals
ation capacity [35]. Besides, for fly ashes with similar chemical com­ ●High pressure (2.0
positions, the smaller the fly ash particles, the higher the carbonation MPa) and
efficiency and capacity [60]. This is because (i) particles with small sizes temperature (220 oC)
[106] Aqueous 7.18% 86.4 % ● Low-calcium fly
have a large specific surface area for carbonation reactions, and (ii) the
ash with 9.2 % CaO
small particle size facilitates the release of metal (Ca2+/Mg2+) ions [64, ●Mean particle size
104,105]. between 20-150 µm
To accelerate the mineral CO2 sequestration of fly ash, most previous ●Brine mixed in
studies had used aqueous carbonation, as listed in Table 2. On that basis, aqueous carbonation
instead of pure tape
to further enhance the carbonation capacity and efficiency of fly ash,
water
aqueous carbonations exposed to different temperatures were investi­ [107] Aqueous 8.81% - ●Fly ash with 15.7 %
gated. In [60], it was noted that the increase in temperature from 20 to CaO
80 ◦ C significantly accelerated the speed of aqueous carbonation of fly ●Carbonation
ash, but the final CO2 uptake capacity only increased slightly (see Fig. 6). duration of 240 h
[108] Aqueous 26.4 % - ●High-calcium fly
Such a phenomenon may be explained in the light of Fig. 5: the tem­ ash (30 % CaO) with
perature rise from 20 to 80 ◦ C improves kinetic energy of carbonation high mass percentage
reactions, leading to the fast speed of CO2 uptake [114]. Meanwhile, the of MgO (25.8 %)
accelerated leaching of calcium ions caused by the temperature rise is ●Particle size
between 2.2-10.0 µm
moderated by the fast formation of calcite layers, resulting in a mild
●Pressure of 1.0 MPa
increase in the final CO2 uptake capacity. In [104], it was reported that [109] Aqueous 5.03 % 67.9 % ●Low-calcium fly ash
as carbonation temperature increased from 100 to 220 ◦ C, the speed and Gas-solid (Aqueous) (Aqueous) (6.74 % CaO) with
capacity of CO2 sequestration of fly ash in aqueous carbonation were 2.63 % (Gas- 35.5 % (Gas- maximum particle
improved substantially. This may be because the sharp increases in the solid) solid) sizes of 1.0 mm
[102] Gas-solid 6% 28.7 % ●High-calcium fly
leaching of mineral ions (Ca2+/Mg2+) and kinetics of carbonation re­ ash (28.42 % CaO)
actions at elevated temperatures overwhelm the delayed effect induced ●High temperature
by the formation of calcite layers. In [102], a similar temperature effect of 600 oC
was also measured in dry carbonation of fly ash. As the carbonation [110] Gas-solid 20.7 % - ●Flue gas containing
both CO2 and SO2
temperature rose from 300 to 600 ◦ C, both the carbonation speed and
from coal-fired power
capacity increased evidently [102].
(continued on next page)
Different from the above analyzed temperature effect, though rising

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L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Table 2 (continued ) capacity. For those slags with similar particle sizes but different mi­
Ref. Carbonation Carbonation Carbonation Remarks crostructures, the larger the specific surface, the higher the carbonation
approach capacity efficiency activity and the higher the potential CO2 uptake capacity [48,105,122,
plants used for
127]. Fig. 7 presents the relationship between the CO2 uptake and
carbonation of fly ash particle size of slag measured in [64]. With the particle size reducing
[111] Gas-solid 18.2 % 74 % ●High-calcium fly from 1000 to approximately 80 µm, the CO2 uptake of the slag was
ash (31.9 % CaO) found to increase exponentially (see the grey trend line in Fig. 7). Then,
● Particle size lower
with the further reduction in the particle size, the CO2 uptake capacity
than 212 µm
●Carbonation decreased. Two possible reasons may explain the decreased CO2 uptake:
temperature of 45 oC (i) the accelerated carbonation reactions of slag caused by reducing
[112] Gas-solid 11.7 % 48 % ●High-calcium fly particle sizes is counterbalanced by the fast formation of the calcite layer
ash (35 % CaO) (as illustrated in Fig. 2); and (ii) the reduced particle size promotes the
●Particle size
between 2-6 µm
dissolution of silicate phases and subsequent incongruent precipitation
●Carbonation of amorphous silica gel on the surface of slag particle which hinders
temperature of 160 further carbonation reactions (similar to the calcite layer) [64].
o
C After carbonation treatment, the size of slag particles tends to
Note: The low-calcium fly ash corresponds to the CaO content less than 8 % (by become coarser due to the formation of amorphous calcite layer un­
mass), whereas the high-calcium fly ash represents the high CaO content over 20 evenly attached to the surface of slag, as illustrated by Fig. 8. Moreover,
% [113]. the density and specific surface area of slag after carbonation appear to
reduce, but its particle cylindrical crushing strength increases
[135–138]. To achieve the maximum potential of CO2 sequestration of
slag, temperature control in carbonation treatment is crucial [46,114,
133], as highlighted in Sections 3.1 and 3.2. In [46], it was reported that
with temperatures rising from 20 to 50 ◦ C, both the rate and capacity of
CO2 uptake of slag were increased. However, the continuous increase in
the temperature from 50 to 80 ◦ C seemed to slightly decrease the ca­
pacity of CO2 sequestration [46]. A similar phenomenon was also ob­
tained in [133] in which the aqueous carbonation experiments of slag
were performed at temperatures ranging between 30 and 80 ◦ C. The
measured CO2 sequestration capacity of slag peaked at approximately
60 ◦ C. The slight decrease in the CO2 sequestration capacity after 50 or
60 ◦ C in [46,133] can be attributed to the rapid growth of the calcite
Fig. 6. Influence of temperature on CO2 sequestration of fly ash, data
layers on the surface of slag particles, as discussed in Sections 3.1 and
from [60].
3.2. In [55], rising temperature from 350 to 600 ◦ C was found to
significantly boost the CO2 sequestration capacity of slag. This demon­
pressure can promote CO2 solubility in liquid (see Fig. 4) and speed up strated that the retarded CO2 sequestration capacity of slag caused by
the rate of carbonation reactions, the final CO2 uptake capacity and the calcite layers can be overwhelmed by the accelerated reaction ki­
efficiency of fly ash tend to be less affected [58,60,103]. Because the netics and the fast leaching of calcium ions at elevated temperatures, as
diffusion of calcium ions and kinetics of carbonation reactions are introduced in the carbonation treatment of fly ash in Section 3.2.
hardly affected by pressure changes that determine the overall CO2 In [46], the effect of pressure changes on CO2 sequestration of slag
sequestration capacity [46,115]. Such an explanation can also be used to was studied within the range between 1.0 and 6.0 MPa. High pressure
explain the influences of the rate and concentration of CO2 flow on was found to accelerate the CO2 sequestration rate at the early stage of
aqueous carbonation of fly ash [59,68]. Besides, the liquid (water)-­ aqueous carbonation but hardly affect the final CO2 sequestration ca­
to-solid (fly ash) ratio can also impact carbonation effect of fly ash in pacity of slag, which is consistent with the effect of pressure on the CO2
aqueous carbonation [60,68,103,106,109,116]. In principle, under a uptake of fly ash (as introduced earlier). In [114], it was proved that the
specific temperature and pressure condition, the determination of the influences of pressure and CO2 concentration on CO2 sequestration of
optimal liquid-to-solid ratio should refer to the solubility and chemical slags were coupled, as shown in Fig. 9. Under a low pressure of 0.1 MPa,
compositions of fly ash [117]. Increasing the concentration of calcium rising CO2 concentration from 10% to 100% tends to steadily accelerate
ions in a fixed aqueous volume can speed up the rate of mineral CO2 CO2 sequestration of BOF slag. However, such monotonous enhance­
sequestration and obtain a high CO2 uptake capacity [118]. ment of the CO2 sequestration with rising CO2 concentration does not
exist at a high pressure of 1.0 MPa. Besides, it can be observed that the
3.3. Slags increase of temperature from 20 to 50 ◦ C improved the overall CO2
sequestration of slag more significantly than the subsequent tempera­
Slags, including, e.g. ground-granulated blast-furnace slag and steel ture rise from 50 to 100 ◦ C. Such temperature effect is in good agreement
(making) slag, as calcium-rich but hydration-inactive materials had with the findings reported in [46,133].
been investigated as desirable candidates for mineral CO2 sequestration In addition to the direct carbonation treatment of granulated slag (as
[119–123], as listed in Table 3. For the same slag, the aqueous introduced above), the other way of using slag as a candidate for mineral
carbonation tends to present considerably higher CO2 sequestration CO2 sequestration is to carry out carbonation treatment of slag compacts
capacity than the gas-solid carbonation [115], as observed in the car­ [140–145]. The manufacturing process of slag compacts is given as
bonations of RCA and fly ash (see Sections 3.1 and 3.2). Under the same follows:
carbonation condition, the CO2 sequestration capacity and efficiency of
slags are closely related to its chemical compositions, particle sizes, and ▪ Pre-treatment of slags: Raw steel slag materials are transferred
microstructures [67,124–126]. The chemical composition of slags de­ into fine slag powders by grinding and then classified by sieving
pends mainly on the steel and iron making process which is also an [65,140,144,146].
important factor affecting its CO2 reactivity [67]. Generally, high CaO
content and small particle sizes can contribute to high CO2 sequestration

6
L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Table 3
Carbonation treatment of slags exposed to varied carbonation conditions.
Ref. Slag type Carbonation Carbonation Carbonation Remarks
conditions efficiency capacity

[46] GGBF slag Aqueous 8.83 % 2.95 % ●Slag with CaO content of 42.5 %
●Up to 50 % of slag particles less than 10 µm
[55] Steel slag Gas-solid 55.5 % 8.85 % ●Slag with CaO content of 39.68 %
(no specific ●Mean particle sizes of 1.62 µm
information) ●Carbonation temperature of 600 oC
●Flue gas for carbonation treatment containing SO2
[64] BOF slag Aqueous 72 % 46.5 % ●Slag with calcium composition of 31.05 %
●Average particle size between 38-63 µm
●Temperature of 50 oC and pressure of 0.5 MPa
[114] BOF slag Aqueous - 5.36 % ●Slag with calcium composition of 31 %
●Average particle sizes between 63-100 µm
●Temperature of 100 oC and pressure of 0.5 MPa
[125] AOD slag Aqueous - 26.0 % (AOD) ●Similar CaO content in AOD and LM slags
LM slag 31.0 % (LM) ●Mean particle size of AOD slag between 20-110 µm
●Mean particle size of LM slag between 3-100 µm
[126] EAF slag Aqueous 50 % (EAF) 18.0 % (EAF) ●EAF slag with calcium composition of 35.2 %
AOD slag 70 % (AOD) 30.0 % (AOD) ●AOD slag with calcium composition of 40.3 %
●Maximum particle size of EAF and AOD slags both below 150
µm
[127] LD slag Gas-solid 35 % 1.5 % ●Mean particle size of slag between 2-3 mm
●Carbonation pressure of approximately 0.02 MPa
[128] EAF slag Aqueous - 1.74 % (EAF) ●EAF slag with CaO content of 32.8 %
LF slag 24.7 % (LF) ●LF slag with CaO content of 58.1 %
●Particle sizes of EAF slag between 315-630 µm
●Particle sizes of LF slag between 160-315 µm
[129] Steel slag Aqueous - 21.1 % ●Slag with CaO content of 40 %
(no specific ●Particle sizes between 38-250 µm
information) ●Temperature of 60 oC and pressure of 1.0 MPa
●Using NH4Cl as the leaching solution of slag
[130] EAF slag Gas-solid 3.7 % (Gas-solid) 1.1 % (Gas-solid) ●Slag with CaO content of 28.27 %
Aqueous 26.97 % (Aqueous) 8.2 % (Aqueous) ●Maximum particle size of around 2 mm
[131] BOF slag Aqueous 93.5 % 29.0 % ●Slag with CaO content of 42.43 %
●Average particle size about 63 µm
●Temperature of 65 oC and pressure of 0.1 MPa
[132] BOF slag Aqueous - 40.0 % ●Slag with calcium composition of 21.3 %
●Average particle size below 125 µm
●Temperature of 100 oC and pressure of 1.0 MPa
[133] BOF slag Aqueous 68 % 27.0 % ●Slag with CaO content of 51.11 %
●Average particle size below 14.98 µm
●Carbonation pressure of approximately 0.1 MPa
[134] BOF slag Aqueous 82 % (BOF) 40.3 % (BOF) ●BOF Slag with calcium composition of 22 %
EAF slag 60 % (EAF) 28.0 % (EAF) ●EAF Slag with calcium composition of 35 %
●Average particle size of BOF slag of 21.5 µm
●Average particle size of EAF slag of 46.5 µm
●Temperature of 100 oC and pressure of 1.0 MPa

Note: EAF Slag - Electric Arc Furnace Slag; AOD Slag - Argon Oxygen Decarburization Slag; LF Slag - Ladle Furnace Slag; LM Slag - Ladle Metallurgy Slag; BOF Slag -
Basic Oxygen Furnace Slag; GGBF Slag - Ground-granulated Blast Furnace Slag; LD Slag - Linz Donawitz Slag.

▪ Shaping of slag compacts: After mixing with water at a specified

liquid-to-solid ratio, fine slag powders are compacted to shaped
granules at a given pressure [119,142,144,147,148].
▪ Carbonation treatment of slag compacts: The obtained slag
compacts are cured for CO2 sequestration right after demolding
[65,119,140,144]. Qualitatively, the higher the CO2 uptake,
the higher the compressive strength of the compacts [144,145,
148]. After carbonation treatment, the slag compacts are then
crushed to angular-shaped granules fitting a gradation for fine
aggregates. Subsequently, a secondary carbonation treatment
can be imposed on the crushed slag compacts.

Generally, the carbonation treatment of slag compacts is performed

Fig. 7. Relationship between the CO2 uptake capacity and particle size of basic
oxygen furnace slag (the red square points represent the experimentally
measured data in [64]).
through gas-solid carbonation. Therefore, pre-carbonation of slag com­
pacts can refer to that of RCA. Due to relatively larger sample sizes, the
CO2 uptake capacity of slag compacts tends to be far lower than that of
the milled slag powders (as listed in Table 3). Despite restrained CO2
sequestration capacity, carbonation treatment still can significantly
affect the properties of slag compacts as substitutes for aggregates in
concrete production [119,145,149].

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L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Fig. 8. Scanning electron micrographs of (a) untreated and (b) carbonated slags
adapted from [139].

Table 4
Main carbonation features of concrete slurry waste, waste gypsum, and cement
kiln dust.
Materials Main carbonation features

Concrete slurry ■Mass percentage of CaO between 32.38% and 37.38%[155,

waste 157] and a much high level of 52.81%[95]
■CO2 uptake capacity of 204.35 g CO2/kg concrete slurry waste
[95]
■CO2 uptake capacity of 110 g CO2/kg concrete slurry waste
[155]
■Carbonation efficiency between 29.7% and 35.2%[155]
Waste gypsum ■CaSO4 as main mineral phase[51,153,158,159]
■Typical mass percentage of CaO between 27.0% and 33.0%
[51,158,159]
■CO2 uptake capacity of between 110 and 250 g CO2/kg waste
gypsum[51]
■Carbonation efficiency of approximately 86.7%[160] and
75–97%[159]
Fig. 9. Coupling effects of CO2 concentration and pressure on carbonation of Cement kiln dust ■Typical mass percentage of CaO between 38.0% and 50.0%
slag, data from [114]. [70,152,156]
■CO2 uptake capacity of between 86.8 and 116.8 g CO2/kg
cement kiln dust[63,156]
3.4. Other waste materials
■Carbonation efficiency of approximately 70.5%[156], 81%
[70], and 70.6–94.3%[63]
Apart from RCA, fly ash, and slags, other industrial wastes were also ■Low hydraulic reactivity but high carbonation reactivity[154]
identified as suitable candidates for carbonation treatment prior to their
utilizations as raw ingredient materials in concrete [95,150–154],
4. Utilization of carbonated industrial waste materials
including concrete (or cement) slurry waste, waste gypsum, and cement
kiln dust. Compared to research on fly ash and slag, studies on carbon­
4.1. As substitutes for aggregates
ation treatment of these three materials remain limited. In terms of
carbonation features of these materials, some key information is sum­
The use of carbonated RCA as replacements for natural aggregates or
marized in Table 4. Similar to high-calcium fly ash and the majority of
untreated (original) RCA has been considered as one of the effective
slags introduced in Sections 3.2 and 3.3, all the three waste materials
approaches contributing to the sustainable development of the concrete
have high content of CaO (over 25%, by mass), indicating great potential
industry. According to [50,161–163], the cement-based composites with
for mineral CO2 sequestration. By the accelerated aqueous carbonation
carbonated RCA tend to exhibit lower drying shrinkage and autogenous
in [95], the CO2 uptake capacity of grained concrete slurry waste was
shrinkage and better chloride penetration resistance in contrast to the
measured at 20.4%, whereas the CO2 uptake capacity was determined at
reference samples with untreated RCA. In [81,84,86,88,164,165], the
11.0% using accelerated gas-solid carbonation in [155]. In [51,63,70,
compressive and tensile strength of cement-based composites containing
156], the CO2 uptake capacity of waste gypsum and cement kiln dust
carbonated RCA were measured. Typically, the incorporation of
was estimated between 11% and 25% and between 8.68% and 11.68%,
carbonated RCA as a substitute for untreated RCA could improve the
respectively. It is obvious that waste gypsum and cement kiln dust both
strength of cement-based composites [96,166,167], though the
could reach a high carbonation efficiency (more than 70%) due to their
improved strength was still slightly lower compared to the control
high carbonation reactivity. For different concrete slurry wastes under
sample with natural aggregates [168,169]. Mechanisms behind the
gas-solid carbonation, their carbonation efficiencies varied between
strength enhancement induced by carbonated RCA are due mainly to (i)
29.7% and 35.2% [155], depending mainly on chemical compositions.
improved physical properties of RCA after carbonation (reduced
Besides, it should be noted that because the main mineral phase of waste
porosity and increased strength) and (ii) reinforced interfacial transition
gypsum is calcium sulfate (CaSO4), ammonia solution (rather than pure
zones between mortar and carbonated RCA [86,88,165,167,170]. To be
water) is usually used to perform aqueous carbonation of gypsum.
more precise, the latter mechanism can be detailed as follows: the calcite
and silica gel formed on the surface of RCA after carbonation treatment

8
L. Li and M. Wu
reacts with the hydration products of the new mortar, forming addi­
tional C-S-H gel [85,88]. Moreover, the chemical reactions between the
carbonation products and new mortar are closely related to the
carbonation degree of RCA. In [84], RCA subjected to different
carbonation conditions (namely, RCA1–4, as shown in Fig. 10) were
employed to create concrete mixtures with a fixed mass percentage of
RCA of 30%. REF stands for the reference concrete containing 30%
untreated RCA, whereas C-RCA1 to C-RCA4 are four mixtures with
carbonated RCA. As plotted in Fig. 10, all concrete with carbonated RCA
present higher tensile strength than REF, but two mixtures (C-RCA3 and
C-RCA4, see Fig. 10(a)) show the decreased compressive strength. The
reason resulting in the decrease in the compressive strength was
attributed to the over-intensified carbonation of RCA under high pres­
sure [84]. In [88], a similar finding was also noted, demonstrating that
over-intensified carbonation would limit the reinforcement of the
interfacial transition zones between new mortar and carbonated RCA.
To sum up, it is evident that RCA exposed to varied carbonation con­
ditions tend to have different influences on concrete properties [84,88,
96].
In addition, the utilization of carbonated slag grains or compacts as a
substitute for natural sands or large aggregates also attracts a great deal
of research interest [119,145,171–174]. Carbonation treatment can not
only greatly deplete CaO in slag contributing to increased volume
Fig. 10. 28-day (a) compressive strength and (b) tensile strength of concrete
containing RCA carbonated at varied conditions
data from [84].
9
Journal of CO2 Utilization 60 (2022) 102000
stability but also reduce the leaching of heavy metals improving its
grindability [121,125,141,175–177]. In [171], it was found that using
carbonated steel slag as a substitute for untreated slag aggregates in
concrete could improve the compressive strength at 7, 28, and 60 days.
Briefly, the enhancement in the compressive strength can be attributed
to two main reasons (similar to RCA): (a) accelerated carbonation im­
proves the bearing strength and particle cylindrical crushing strength of
granular slag [138], and (b) carbonated slag particles can form much
stronger interfacial transition zones than untreated slag aggregates
[171]. Besides, autogenous deformation of concrete with carbonated
slag aggregates was studied in [178]. Due to an internal curing effect,
the incorporation of carbonated slag as replacement for natural aggre­
gates significantly mitigated the evolution of autogenous deformation.
In [172], concrete samples with carbonated slag aggregates were noted
to have stronger freeze-thaw resistance compared to reference samples
with natural aggregates.
4.2. As supplementary cementitious materials
After carbonation treatment of industrial waste materials, the other
brilliant utilization of the carbonated materials is the incorporation into
the production of concrete as substitutes for Portland cement. Although
research on such utilization remains limited, the initial outcomes ob­
tained in existing studies have presented a bright and encouraging
outlook. In [68,179], it was reported that the early-age compressive
strength of mortars containing 10% carbonated fly ash as a partial
replacement of cement was comparable with that of mortars without fly
ash. In [180], the inclusion of carbonated fly ash as a replacement for
untreated fly ash (without carbonation) was found to effectively in­
crease the compressive strength of mortars at early ages. Besides, Sahoo
et al. observed that concrete with carbonated fly ash as supplementary
cementitious materials demonstrated strong resistance against salt,
sulfate, and acid attack [181]. In [182], the mechanical properties of
cement pastes and mortars with carbonated slag as a cement substitute
were investigated. It reported that with the mass percentage of
carbonated slag rising from 10% to 50% (as replacement of cement),
cement pastes with carbonated slag all maintained great volume sta­
bility. Compared to reference samples containing 10% of untreated slag,
mortars with 10% carbonated slag showed a lower porosity and much
higher 28-day compressive strength. Similar findings were also noted at
7 and 56 days in [183]. To sum up, the positive influence of carbonated
fly ash and slag on the strength gain of cement pastes and mortars can
result from (i) the fine calcite particles produced in carbonation treat­
ment [184] fills the pores of mortars and thereby reduces the porosity
[179,182]; and (ii) the produced calcite reacts with aluminate (C3A),
contributing to the formation of calcium carboaluminate phases [148,
179,182,183,185].
Fig. 11. shows the measured 28-day compressive strength of mortars
containing untreated or carbonated BOF slags with different CO2 uptake
in [182]. It is clear that all mortar samples containing carbonated slag
(10%, by mass of cement) present enhancement in the compressive
strength compared to the reference samples with 10% untreated slag
(CO2 uptake equal to 0). However, the incorporation of significantly
carbonated slag (CO2 uptake higher than 13%) in mortars reduces the
strength enhancement. A similar conclusion was also obtained in [183]
in which the mortar samples with slag carbonated for a long period
showed a low compressive strength gain at 56 days. This may be because
(a) deep carbonation treatment weakens the chemical reactivity of
carbonation products and thereby hinders the reaction between the
carbonation products and cement paste (as introduced earlier); and (b)
deep carbonation further lowers the pozzolanic reactivity of slag [180,
182,186].
After grinding and sieving processes, untreated concrete slurry
waste, waste gypsum, and cement kiln dust (without carbonation) were
also used as supplementary cementitious materials in previous research
[152,154,155,187]. However, using these waste materials as partial
L. Li and M. Wu
Fig. 11. Compressive strength of mortars containing untreated or carbonated
BOF slags with different CO2 uptake
data from [182].
replacement of cement tends to dramatically reduce the strength and
durability of cement-based composites [95,154,188]. Regarding the
employment of those waste materials after carbonation, limited research
has been carried out. As a good reference, the incorporation of
carbonated concrete slurry waste in mortar as a new supplementary
cementitious material was studied in [95]. It was found that using
carbonated concrete slurry waste instead of untreated concrete slurry
waste could improve the compressive strength of mortars at 7 and 28
days [95]. The mechanisms behind the strength improvement can refer
to studies of fly ash and slag. Through the analysis above, key advan­
tages and disadvantages from the technical viewpoint of using industrial
waste materials with and without carbonation treatment in concrete can
be summarized, as briefed in Table 5.
5. Accelerated carbonation of cement-based composites at early
ages
For the carbonation curing of cement-based composites at early ages,
gas-solid carbonation is often used [10,37,43,189]. Generally, the
carbonation curing of fresh cement-based composites at fluid state ap­
pears to be less effective [20,57,94], due to the blocked diffusion of CO2
by liquid. From the hydration accelerating period of cement paste on­
wards, with substantial production of calcium hydroxide and C-S-H
taking place, the cement-based composites become ready for carbon­
ation [94]. Therefore, carbonation curing is usually carried out after a
period of conventional curing (as shown in Fig. 12). In practice, the
duration (T1) of the conventional curing can directly affect the effect of
the followed carbonation curing and the mechanical properties of
cement-based composites [37,39,44]. Typically, prolonged conven­
tional curing after casting can mitigate the CO2 uptake capacity and
speed of the followed carbonation treatment [39], while too short
conventional curing tends to impair the strength evolution of
Table 5
Key advantages and disadvantages of using carbonated/uncarbonated waste
materials in concrete.
Advantages of using industrial waste Disadvantages of using industrial waste
materials with carbonation treatment materials without carbonation treatment
● Increased volume stability ● Reduced compressive and tensile
● Reduced leaching of heavy metals strengths
● Improved strength properties ● Poor durability
● Enhanced resistance against salt, ● Undesirable volume expansion
sulfate, and acid attack
10
Journal of CO2 Utilization 60 (2022) 102000
cement-based composites [37]. For simplicity, the focus of the current
work is mainly on the effect of carbonation curing on the early-age
properties of plain cement-based composites without any re­
inforcements (e.g. fibers and polymers). Although the recent publica­
tions on fiber reinforced cement composites are noted, they are not
further explored in this work. For cement-based composites with or
without reinforcements, the mechanisms behind the carbonation of pure
cement matrix are essentially the same.
In the literature, many researchers believe that proper carbonation
curing can contribute to high early-age strength and rapid strength gain
of cement-based composites, due primarily to the microstructure
densification associated with the pore filling effect by calcite particles
produced in carbonation curing [21,36,40–42,189,190], see Fig. 13. In
fact, besides the decrease in porosity, other effects responsible for the
rapid strength gain after carbonation can be attributed to (a) the for­
mation of amorphous calcium carboaluminate phases (as introduced in
Section 4.2) [148,179,182,183,185], and (b) the presence of the
newly-formed calcite particles (in carbonation) as nucleation sites for
C-S-H gel growth of cement paste [41,95,191]. However, it should be
noted that prolonged or over-intensified carbonation curing tends to
inferior the development of compressive strength at early ages [20,21,
39,40]. The negative effect may result from (i) retarded cement hydra­
tion by carbonation curing [37,39]; (ii) decalcification of C-S-H [39,97,
192,193]; (iii) cracking of microstructures induced by carbonation
shrinkage [21,194]; and (iv) consumption of C2S in carbonation curing
retarding the strength gain of cement pate at late ages [118,195]. For a
given concrete mixture, there may exist a CO2 uptake threshold over
which prolonged (or over-intensified) carbonation curing at early ages
appears to be deleterious [20]. Consequently, a balance should be
sought for early-age carbonation of cement-based materials that maxi­
mizes CO2 uptake, yet without compromising the mechanical and
long-term durability performance.
6. Discussion
6.1. CO2 sequestration potential of industrial waste materials
Theoretically, the mineral CO2 sequestration capacity of industrial
waste materials is proportional to the elemental content of calcium. In
fact, the carbonation reactivity of minerals is affected not only by the
content of calcium but also by the mineral phases in which the calcium
ions are fixed [196]. Typically, the existence of calcium carbonate and
calcium phosphate in materials contribute to high calcium composition
but cannot participate further in accelerated carbonation reactions
[196]. Based on the realistically measured data summarized in
Tables 2–4, the variation of the CO2 uptake capacity over the mass
percentage of CaO content of industrial waste materials was assessed, as
plotted in Fig. 14(a). With the CaO content increasing, the mineral CO2
sequestration capacity of the minerals appears to show an overall rising
trend. Ordinary Portland cement with a typical CO2 uptake capacity of
approximately 30% and CaO content of around 65% provides a bench­
mark for assessing the carbonation capacity of the waste minerals.
Roughly, slag, cement kiln dust, waste gypsum, and concrete slurry
waste present the comparable potential for mineral CO2 sequestration.
Besides, fly ash with high calcium content (over 20% by mass) can also
be regarded as a great candidate for CO2 sequestration, while other fly
ash that is lacking in calcium only has mild carbonation capacity. Fig. 14
(b) displays the carbonation efficiency of the industrial waste materials
listed in Tables 2–4. It can be observed that the carbonation efficiency of
materials appears to be less linked to the CaO content, indicating that
the main factors affecting the carbonation efficiency are the particle
sizes and microstructures of the materials and accelerated carbonation
conditions. It is of interest to note that waste gypsum and cement kiln
dust seem to have an overall higher carbonation efficiency (see the area
enclosed by dotted lines) than other materials.
L. Li and M. Wu Journal of CO2 Utilization 60 (2022) 102000

Fig. 12. Accelerated carbonation curing of cement-based composites at early ages (T1 and T2 represent the duration of the conventional curing and carbonation
curing, respectively).

Fig. 13. Scanning electron micrographs of cement paste at an age of 28-day (a) without accelerated carbonation and (b) subjected to carbonation between ages of 24
and 28 h
adapted from [36].

Fig. 14. Comparisons of the carbonation (a) capacity and (b) efficiency of in­
dustrial waste materials.
6.2. Optimization of accelerated carbonation treatment
Based on the data analysis in Section 3, it can be noted that in
aqueous and gas-solid carbonation, CO2 flow with high concentration
appears to be not necessary for achieving a high CO2 uptake of materials.
The direct use of waste flue gas instead of pure CO2 in carbonation
treatment seems to be acceptable [55,110,197,198]. In reality, the uti­
lization of waste flue gas is of considerable significance for promoting
the development of accelerated carbonation at an industrialized scale.
Because such utilization not only reduces energy consumption but also
increases economic viability. So far, some waste flue gases indeed have
shown great potential for conducting accelerated carbonation treat­
ment. Generally, the typical CO2 concentration of waste flue gas from a
cement plant is around 14–33%, whereas that from an iron and steel
plant is between 20% and 30% [9,91]. Such CO2 concentration of the
waste flue gases is desirable for performing carbonation treatment in the
concrete industry [96,197,198].
Temperature is one of the most crucial parameters affecting both gas-
solid and aqueous carbonation of materials. Among all those parame­
ters, the effect of temperature is indeed the most complicated. Because
the leaching of metal (mainly Ca2+) ions, the dissolution of HCO3-/CO32-
ions, the kinetics of carbonation reactions, and the precipitation of
carbonation products (calcite) all are simultaneously affected by tem­
perature [48,64,133]. To reach economical CO2 sequestration, a ma­
jority of previous research practiced carbonation treatment of
construction materials between 20 and 80 ◦ C (as analyzed in Section 3).
In such a temperature scope, with the carbonation temperature rising,
the CO2 sequestration capacity of the materials tends to increase.
Although some studies reported that the highly elevated temperature
from 100 –140 ◦ C to 300–600 ◦ C would further improve the CO2 uptake
capacity of materials [55,102,104], lots of technological barriers for
using high temperature at an industrial scale have not been addressed.
In addition, through the analysis in Section 3, it can be summarized
that the influence of high pressure on accelerated carbonation is due
mainly to the impact of increased pressure on the accelerated dissolution
of HCO3-/CO32- ions in liquid. According to Henry’s law [199,200], at a
given temperature the concentration of CO2 that dissolves in liquid is
directly in proportion to the partial pressure of CO2 above the liquid.

11
L. Li and M. Wu
Yet, the leaching of metal ions (Ca2+/Mg2+) and kinetics of carbonation
reactions are less affected by pressure change. This implies that rising
pressure may speed up the rate of CO2 sequestration but is irresponsible
for the increase in the carbonation capacity and efficiency of materials
[111]. Besides, from the viewpoint of energy conservation, accelerated
carbonation treatment performed at high temperature or high CO2
concentration may not necessarily require high pressure (as discussed in
Section 3).
6.3. Environmental impact of accelerated carbonation treatment
To apply mineral CO2 sequestration at a commercial scale, the
environmental impact of accelerated carbonation treatment must be
considered, since the energy consumption required as an input to
accelerate carbonation reactions is usually significant. To quantify the
environmental impact, a life cycle assessment can be conducted, e.g. see
[14,92,139,201,202]. In this section, the Global Warming Potential
(GWP) that represents the amount of greenhouse gas emissions with the
unit of kg CO2 eq. per kg of the material was used as the main indicator
of assessing the environmental impact of producing carbonated
materials.
Fig. 15 illustrates the reported GWP data for manufacturing different
construction materials (excluding accelerated carbonation treatment). It
can be noted that the manufacture of 1.0 kg of cement usually generates
0.84–0.95 kg of CO2 [80,201,203–205], which is far higher than the
GWP of fly ash and slag (0.004 and 0.083 kg CO2 eq./kg [75,204],
respectively). Besides, the production of RCA tends to have slightly
higher CO2 emissions than that of natural aggregate (0.003 kg CO2
eq./kg [76,80]). Obviously, using fly ash and slag as substitutes for
cement is environmentally friendly, whereas employing RCA as a
replacement for natural aggregate may not have significant influence on
the CO2 emissions of concrete [206,207]. Despite substantial previous
research, GWP values of RCA, fly ash, and slag after accelerated
carbonation treatment remain absent. Generally, the electricity con­
sumption during the accelerated carbonation process is the biggest
contribution to the increased CO2 emissions in the production of
carbonated materials. The typical GWP of electricity is between 0.34 and
0.95 kg CO2 eq./kWh, as listed in Table 6. In practice, the amount of
electricity consumption is closely related to carbonation conditions
(carbonation duration, pressure, temperature, etc.) and facilities. In
terms of the GWP of RCA and other industrial waste materials subjected
to accelerated carbonation treatment, systematic research and reliably
measured data are still few. Accordingly, the following discussion fo­
cuses mainly on the determination of GWP of fly ash and slag in accel­
erated carbonation treatment.
For the accelerated gas-solid carbonation of slag in [65], the GWP
was estimated at about 0.208 kg CO2 eq./kg slag. The determined CO2
uptake of the slag was around 0.09 kg CO2/kg slag. Consequently, the
net GWP for carbonating the slag was 0.118 kg CO2 eq./kg slag,
demonstrating that the gas-solid carbonation treatment of the slag was
Fig. 15. Typical GWP values of different construction materials
data from [75,76,203–209].
12
Journal of CO2 Utilization 60 (2022) 102000
Table 6
GWP of electricity (unit: kg CO2 eq./kWh).
Ref. [10] [13] [17] [209] [208] Average
GWP 0.75–0.95 0.412 0.41–0.79 0.548 0.343 0.5
carbon positive (CO2 emissions higher than CO2 sequestration). In [15,
60], the electricity consumption for sequestration of 1.0 ton of CO2
through aqueous carbonation of slag and fly ash was measured at 1610
MJ and 1055 MJ, respectively. In accordance with [10,13,17,208,209],
it was hypothesized that the average GWP of electricity was 0.5 kg CO2
eq. per kWh, see Table 6. Combining with the measured CO2 uptake
capacities of the slag (0.20 kg CO2/kg) and the fly ash (0.027 kg
CO2/kg) in [15,60], the GWP of the carbonated slag and fly ash were
approximated at 0.045 kg CO2 eq./kg and 0.004 kg CO2 eq./kg,
respectively. Because the obtained GWP values both are lower than the
corresponding CO2 uptake, the accelerated carbonation treatments in
[15,60] are therefore carbon negative (CO2 sequestration higher than
CO2 emissions). In [134], the energy requirements for 1.0 ton CO2
sequestration via aqueous carbonation of the slag was estimated be­
tween 1350 and 2200 MJ. The CO2 uptake capacity of the slag was
determined at 0.403 kg CO2/kg. On that basis, the GWP of performing
carbonation for the slag was approximated between 0.077 and 0.125 kg
CO2 eq./kg, which was less than the CO2 uptake of the slag. Therefore,
the accelerated carbonation of the slag in [134] was carbon negative.
The same conclusion was also reported by Ghasemi et al. in [209].
In the analysis above, it should be noted that all determined GWP
results are based mainly on experimental results measured in the labo­
ratory, due to the lack of data from industrially used carbonation test
setups. Particularly, the energy consumption in transportation of slag
and fly ash is not properly considered in the estimation of GWP.
Consequently, the approximated GWP values may underestimate the
actual greenhouse gas emissions in practice.
6.4. Remaining issues in accelerated carbonation treatment of
construction materials
In previous research, the effect of temperature on accelerated
carbonation curing of industrial waste materials had been investigated,
but a comprehensive understanding of the temperature effect remains
absent. For industrial waste materials with different chemical compo­
sitions, particle sizes, and microstructures, the effect of temperature on
the carbonation of the materials tends to vary. Substantial studies
indicated that rising temperature from ambient temperature to a
threshold value of between 60 and 80 ◦ C would improve both the CO2
sequestration capacity and the carbonation speed of materials. Over the
threshold value, a mild increase in temperature seems to hardly affect or
even hinder mineral CO2 sequestration. However, with the temperature
rising continuously, the CO2 uptake capacity and efficiency can be
greatly improved again at elevated temperatures. To systematically
explain the complicated temperature effect, further research is therefore
needed.
Besides, studies on the utilization of carbonated materials as sub­
stitutes for aggregates or cementitious materials in concrete are still few
(as analyzed in Section 4). Most previous studies on accelerated
carbonation treatment of RCA, fly ash, slag, etc. target at exploring
optimal carbonation conditions for maximizing the CO2 uptake capacity
of the materials. However, for a specific material, there may exist a CO2
uptake threshold over which increasing CO2 uptake tends to be delete­
rious for the strength enhancement of the cement-based composites
containing the carbonated material (see Figs. 10 and 11). To combine
pre-carbonation treatment with followed utilizations of the pre-
carbonated materials, the optimum CO2 uptake corresponding to the
most significant strength enhancement should be investigated in-depth.
The influences of early-age carbonation curing on the properties of
cement-based composites have not been fully understood in neither the
L. Li and M. Wu
short term nor the long term due to a number of reasons, including the
complicated coupling effect between carbonation and hydration re­
actions at early ages. Based on the existing research outcomes summa­
rized in Section 5, it is clear that over-intensified carbonation curing at
early ages appears to compromise the mechanical properties of cement-
based composites. To achieve proper control of the accelerated
carbonation curing at a commercial scale and avoid over-intensified
carbonation, a rigorous yet practical assessment system consisting of a
series of quantitative parameters (including CO2 uptake, carbonation
depth, carbonation time, etc.) is therefore needed. To build such an
assessment system, a large amount of research on early-age carbonation
curing of cement-based materials performed under varied carbonation
conditions is in high demand. In addition, it must be noted that sys­
tematical evaluation of the early-age carbonation curing on cement-
based composites with pre-carbonated ingredient materials is
currently missing. This is a research gap hindering the utilization of pre-
carbonated ingredient materials in the concrete industry.
7. Summary and concluding remarks
Mineral CO2 sequestration in the concrete industry has unique ad­
vantages for the mitigation of global greenhouse gas emissions yet
confronts industrial challenges and technological barriers. In the past
few decades, a growing amount of research had paid attention to the
establishment of mineral CO2 sequestration at a commercial scale.
However, due to the complicacy of the accelerated carbonation of
different construction materials and the lack of consistency of previous
studies, the practical utilization of carbonation treatment in the concrete
industry remains limited at present. In this paper, the state-of-the-art
studies of the pre-carbonation of raw construction materials and the
early-age carbonation curing of cement-based composites were
reviewed systematically. In particular, a special focus was laid on the
identification of the remaining critical issues that impede the utilization
of accelerated carbonation in the concrete industry. The key findings
and conclusions reported in the work include:
• To build a comprehensive understanding of the mineral CO2
sequestration process of construction materials, pre-carbonation
treatment of RCA, fly ash, and slags performed under varied
carbonation conditions was analyzed in detail. Influences of the
chemical compositions, microstructures, and particle sizes of the
materials and the carbonation conditions on the mineral CO2
sequestration were summarized. For a given material, particle sizes
and temperature were identified as the most important factors
determining the CO2 sequestration in both aqueous and gas-solid
carbonation. Pressure and CO2 concentration could affect the speed
of mineral CO2 sequestration yet hardly influence the final CO2 up­
take capacity of the material. Besides, the environmental impact of
pre-carbonation treatment of fly ash and slag was approximated, and
the calculated results exhibited that the production of pre-
carbonated fly ash and slag could be carbon negative.
• After pre-carbonation treatment, the inclusion of the carbonated
industrial waste materials (RCA, fly ash, slag, concrete slurry waste,
et al.) in cement-based composites in general tends to be beneficial
for the mechanical properties. However, over-intensified pre-
carbonation treatment (or increasing CO2 uptake) of the materials
would reduce the strength enhancement effect. Similarly, over-
intensified carbonation curing at early ages was also found to be
undesirable for improving the performance of cement-based com­
posites. To explain the mechanisms behind the negative influence of
over-intensified carbonation, four possible reasons were identified,
including retarded cement hydration, decalcification of C-S-H,
cracking of microstructures, and consumption of C2S. When con­
ducting pre-carbonation treatment or early-age carbonation curing
in the concrete industry, it is of considerable importance to seek a
13
Journal of CO2 Utilization 60 (2022) 102000
balance that maximizes CO2 uptake, yet without compromising the
performance of the final products.
CRediT authorship contribution statement
Liang Li: Methodology, Validation, Investigation, Writing – original
draft. Min Wu: Conceptualization, Supervision, Project administration,
Funding acquisition, Writing – review & editing.
Acknowledgments
The authors acknowledge the financial support from the Danish
Offshore Technology Centre, Denmark. Part of this work received sup­
port from COWIfonden, which is greatly acknowledged.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
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