1 s2.0 S0008884623002661 Main

Cement and Concrete Research 175 (2024) 107352
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Cement and Concrete Research

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Carbonate binders: Historic developments and perspectives

Xiang Hu, Pingping He, Caijun Shi *
Key Laboratory for Green & Advanced Civil Engineering Materials and Application Technology of Hunan Province, International Science Innovation Collaboration Base
for Green & Advanced Civil Engineering Materials of Hunan Province, College of Civil Engineering, Hunan University, Changsha 410082, PR China
Key Laboratory of Building Safety and Energy Efficiency of Ministry of Education, Changsha 410082, China
A R T I C L E I N F O A B S T R A C T
Keywords: This paper reviews the historic developments and provides some perspectives of carbonate binders. Various
Carbonate binders carbonatable materials have been used to produce carbonate binders using different carbonation techniques. The
Calcareous materials carbonate binders are mainly composed of calcium/magnesium carbonate and silica/alumina gels. Three crys
Magnesium-based materials
talline polymorphs, namely calcite, aragonite and vaterite can be formed. The properties of carbonate binders are
Industrial by-products
strongly affected by the crystalline polymorphs and also the polymerization degree of amorphous silica gel.
During the past 4 years, physical, chemical and biological methods have been proposed to control the poly
morphous of calcium carbonate. Some industrial demonstration and applications have already been successfully
implemented. The production and application of carbonate binders can use up to several hundred million tons of
CO2. However, there is an urgent need to increase the carbonation degree and to regulate the composition and
structure of carbonate binders so to achieve better performance of carbonated construction products.
1. Introduction Given the substantial development and increased interest in low

carbon materials, the research achievements on carbonate binders
Carbonate binders are produced via reactions between carbonatable together with alkali-activated materials were reviewed in the 15th In
materials and CO2 instead of hydration between calcium silicate/ ternational Congress on the Chemistry of Cement (ICCC 2019) [1].
aluminate with water. Carbonate binders are mainly composed of cal However, due to extensive studies and achievements obtained in the
cium carbonate (CaCO3) and amorphous silica/alumina gel. The car past 4 years, this paper will review the historical development as well as
bonatable materials mainly include calcium or magnesium silicate/ the recent progresses on carbonate binders. The review will cover crit
aluminosilicate or hydroxide phases [1]. The properties and perfor ical aspects, including major carbonatable materials and carbonation
mance of carbonate binders are significantly influenced by the origi processes, an in-depth analysis of the composition of carbonate binders,
nated carbonatable materials and the carbonation techniques and their structure, and performance, and a presentation of their diverse
conditions. Generally, calcareous materials including tricalcium silicate applications. The literature will be assessed and discussed considering
(C3S), β-dicalcium silicate (β-C2S), monocalcium silicate (CS), tricalcium the different carbonatable sources from which the carbonate binders
disilicate (C3S2) and γ-dicalcium silicate (γ-C2S), calcium aluminate originate. Additionally, it will focus on the carbonation technique to
compounds such as tricalcium aluminate (C3A) and/or magnesium produce carbonate binders such as CO2 curing and aqueous mineral
compounds including magnesium oxide and magnesium silicate can be carbonation, and highlight potential research gaps that require further
used to produce carbonate binders. While detailed studies on carbon investigation.
ation of calcium silicates date back to the 1970's [2–5], it wasn't until the
past two decades that research interest in this area rebounded, driven by 2. Historic development of carbonate binders
concerns over greenhouse gas emission. Several reviews of design,
characterization, production and modeling of carbonate binders have The carbonation of alkaline earth hydroxides such as slaked lime or
been published recently [6–11]. dolomitic lime with atmospheric CO2 to form carbonate binders has
* Corresponding author at: Key Laboratory for Green & Advanced Civil Engineering Materials and Application Technology of Hunan Province, International
Science Innovation Collaboration Base for Green & Advanced Civil Engineering Materials of Hunan Province, College of Civil Engineering, Hunan University,
Changsha 410082, PR China.
E-mail address: [email protected] (C. Shi).
https://doi.org/10.1016/j.cemconres.2023.107352
Received 29 March 2023; Received in revised form 30 September 2023; Accepted 18 October 2023
Available online 23 October 2023
0008-8846/© 2023 Elsevier Ltd. All rights reserved.
X. Hu et al. Cement and Concrete Research 175 (2024) 107352
been known for a long time [12]. However, the natural carbonation of resulted in a compressive strength similar to that of the specimens
lime takes long time and demonstrates slow strength development. subjected to 24 h of steam curing at 60 ◦ C [31].
Carbonation can be significantly accelerated when materials are Since then, numerous studies have been published, using the pre-
exposed to high CO2 concentrations and/or pressures. Table 1 provides conditioning method to improve the carbonation efficiency during the
an overview of the key milestones achieved throughout the development production of carbonate binders [32–34]. Shao et al. [35] used fan
of carbonate binders. The production of carbonate binders was firstly drying to partially remove water before carbonation, and the CO2 up
patented by Rowland in 1870 [12], which described a CO2 curing take of light-weight aggregate concrete reached 9.5 % mass percentage
chamber used for accelerating the hardening of concrete products such of cement, which was higher than that without fan drying. El-Hassan
as tubes and pipes. Then, numerous patents emerged in the late 1800's and Shao [36] investigated the effect of pre-conditioning on CO2
and early 1900's for the production of cementitious materials by curing of lightweight concrete masonry units. The CO2 uptake increased
carbonation [13–17]. Over 100 years after the first issued patent, Berger from 8.5 % to 22 % when pre-conditioning was adopted. He et al. [34]
et al. [2] studied the impact of water to cement (w/c) ratio, compaction also compared the content of carbonate binders formed within cement-
strength, CO2 pressure, etc. on the carbonation process. bonded fiberboards with or without pre-conditioning and found that the
In the 1990s, the accelerated carbonation was applied for wood- CO2 uptake increased from 2.5 % to 20 % when the water content
cement board by injecting CO2 into the furnish during pressing, decreased from 100 % to 40 %. In 2018, Sharma et al. [37] used pre-
whereupon the cement sets within a few minutes. CO2 reduced the conditioning to enhance the properties of carbonated cement mortars
pressing time of cement-bonded wood composite boards and decreased containing cement kiln dust. Pre-conditioning has also been used to
the wood-cement incompatibility as well [18,24]. The properties of the improve the carbonation degree of supercritical CO2-cured cement
CO2-cured boards were similar to those cured with conventional cold- [38,39]. The CO2 uptake could reach around 30 % when removing 40 %
pressing method [25]. Similarly, supercritical CO2 (7.5 MPa) was also of water during pre-conditioning process from the precast engineered
used in another study to improve the properties of wood-cement board cementitious composite specimens with a water to cement (w/c) ratio of
[26,27]. Supercritical CO2 decreased the curing time while maintaining 0.58 [40]. If the pre-conditioning process is regulated, formation of
the same properties as those treated with gaseous CO2 (0.5-4 MPa) [28]. carbonate binders can be used for purpose of surface treatment of con
The applied high pressure accelerated the diffusion of CO2 within the crete products [41].
materials, increased the carbonation reaction rate and produced more The pre-conditioning method has also been used to produce car
carbonate binders [29]. These carbonate binders interlocked with wood, bonate binders in several construction materials such as ultra-high
resulting in an excellent strength of the composite. Along with high performance concrete (UHPC) [42], recycled aggregate concrete
pressure and temperature, supercritical CO2 curing accelerated the [43,44], alkali-activated cement [45,46], wood-lime biocomposite [47],
carbonation process; nevertheless, these conditions resulted in a high and MgO-based materials [48], etc. Generally, the carbonatable mate
energy consumption. It is important to highlight that the carbonation of rials is molded and cured or treated in dry gases CO2 environment,
the wood-cement board using supercritical or gaseous CO2 was limited leading to the formation of carbonate binders that could be incorporated
to its surface layer, leading to a low carbonation degree [26]. Similarly, into concrete [31,35]. Besides, carbonation can also take place in
low carbonation degree has been observed in cement-based materials aqueous environment, where the carbonatable compounds, such as
due to the very low diffusion rate of CO2 in the pore solution, which is recycled concrete fine (RCF) and steel slag powders, react with the
approximately 1/10000 of that in the air [30]. As known, the capillary dissolved CO2 in the liquid medium [49]. The aqueous carbonation
pores of cement-based materials, in fresh or hardened states, are fully or process, also known as wet carbonation, is extensively studied recently
partly saturated with water, resulting in high inner relative humidity. It to treat and transform cement waste and industrial by-products into
was not until the mid-2000s that Shi and Wu [31] introduced a novel supplementary cementitious materials (SCMs), as shown in Fig. 2.
pre-conditioning technique, as shown in Fig. 1 to accelerate the diffusion Another area of research interest in carbonate binders is the accel
of CO2 gases into cement-based materials. Their innovative approach erated carbonation of magnesium-based materials [50]. The “micro
involved pre-conditioning the specimens to remove excess of water from aggregate” formed during carbonation played a key role in the
capillary pores prior to CO2 curing, thus enhancing and accelerating the densification of the matrix [51], while the interlocking network struc
CO2 diffusion and consequently achieving a high carbonation degree ture formed by interconnected and well-developed carbonate binders
within a very short period of time. The suggested approach was put into (such as Nesquehonite) controlled the overall performance of carbon
practice by subjecting concrete blocks to 2 h of pre-conditioning under ated MgO cement (CMC).
dry environment followed by 2 h of exposure to gaseous CO2. This The carbonation reaction between CO2 and cement-based materials
is an exothermic reaction. Generally, the carbonation rate is generally
faster than that of hydration rate, especially at the early stage [52].
Table 1 Therefore, early CO2 curing is considered to be efficient to accelerate
Key milestones of technology evolution for production of carbonate binders. and improve the early strength development of concrete products by
Year Authors Contributions References formation of carbonate binders [53,54]. Furthermore, researchers have
confirmed that the carbonate binders formed on the surface of concrete
1870 James L. Carbonate binders produced by CO2 [12]
Rowland curing of concrete blocks
blocks improved their pore structure and decreased their permeability
1972 Klemm and The mechanisms of carbonate binders [2] [41,55,56]. Moreover, wet carbonation has been used to produce SCMs
Berger formation by carbonation of calcium from industrial by-products and cement waste powders [57–59]. The
silicate properties of carbonate binders are as good as or even better than those
1992 Souza M. R. et Application of carbonate binder for rapid [18]
of hydrated binders [52]. Due to the consumption of CO2 gas during the
al production of cement particleboard
1998 Hermawan D, Supercritical carbonation method for [19] production of carbonate binders, their use is considered an efficient
et al production of carbonate binders approach to solidify and utilize CO2 from industrial waste gas [60,61].
2007 Shi and Wu Pre-conditioning of products to speed up [20] Motivated by the energy conservation and carbon reduction policies,
and increase CO2 uptake several companies successfully scaled and marketed carbonate binders
2011 Solidia Carbonate binders from carbonation of [21]
CS and C3S2
and CO2-cured cement based materials [21,62]. Currently, researches on
2018 Shi C. et al CO2 treatment of hardened cement paste [22] carbonate binders are focusing on increasing CO2 sequestration [63],
powder enhancing the performance of carbonate binders and products [64,65],
2021 Carbstone Conversion of calcium rich slag into [23] and conducting life cycle carbon emission analysis [66,67].
building materials by carbonation
2
Fig. 1. Schematic diagram of pre-conditioning and CO2 curing of concrete products.
Fig. 2. Schematic diagram of the wet carbonation of cement waste fines.
3
3. Carbonate binders from calcareous materials cement. Conventional Portland cements contain nearly 80 % of C3S and
β-C2S. The calcium contents in C3S and β-C2S are relatively high and
Calcareous materials are a widely produced and least expensive consume a larger amount of limestone as raw material for their pro
natural and/or synthetic materials, which includes hydraulic calcium duction. Moreover, the calcination temperature for the production of
silicate and calcium aluminate mainly contained in Portland cement, hydraulic calcium silicate compound is high. In an effort to reduce the
and non-hydraulic calcium silicate. It is being used for the production of carbon footprint associated with cementitious materials, there has been
a variety of cementitious materials and products. Extensive researches a growing interest in the production and use of low-lime non-hydraulic
[36,68,69] have been conducted on the carbonation of different calcium silicates such as CS, C3S2 and γ-C2S. Whether they are hydraulic
calcareous materials, especially with Portland cement system. Due to the or non-hydraulic in nature, these calcium silicate compounds exhibit
carbonatable phases in Portland cement, production of concrete prod relatively high reactivity towards carbonation [52]. In addition to cal
ucts by carbonation has been widely investigated and already applied. cium silicate compounds, studies have been conducted on the carbon
Shi et al. [31,70,71] systematically studied the effect of carbonate ation of C3A, C4AF (tetra calcium aluminoferrite) to produce carbonate
binder on the performance of lightweight cement concrete blocks. The binders [75,76].
results showed that CO2-cured blocks demonstrated lower drying
shrinkage and water absorption than steam-cured ones. Pervious con
crete is regarded as a better recipient for CO2 curing due to its highly 3.1. Carbonation of hydraulic calcium silicate
interconnected void content [72,73]. It also shows deeper and more
homogeneous carbonation depth than conventional concrete. Moreover, In 1972, Berger et al. [4] studied the accelerated CO2 curing of hy
the formation of carbonate binders could significantly improve the draulic calcium silicates with a low water-to-solid ratio of 0.1. In a
freeze-thaw and leaching resistance of concrete products. recent study [78], the compressive strength of the carbonated β-C2S
The main anhydrous calcium silicate compounds include tricalcium specimen reached as high as 120 MPa when the carbonation time was
silicate (C3S), dicalcium silicate (β-C2S and γ-C2S), monocalcium silicate prolonged to 168 h. Generally, the carbonation rates of C3S and β-C2S
(CS) and tricalcium disilicate (C3S2). The crystal structure and properties are higher than their hydration rates due to their high heat flow intensity
of different calcium silicate minerals are shown in Table 2 [74]. Among [79,80]. As the major mineral phases contained in Portland cement and
these calcium silicates, C3S and β-C2S with large calcium to silicon (Ca/ other industrial by-products such as steel slag, the carbonation of hy
Si) ratio are hydraulic and can hydrate with water and produce calcium draulic calcium silicate has been extensively studied [4,81,82]. Gener
silicate hydrate (C-S-H) gel, which endorse the setting and hardening of ally, the carbonation of calcium silicate mineral is a dissolution-ion
diffusion-precipitation process. As shown in Fig. 3 [83], in the presence
Table 2
Crystal structure and morphology of calcium silicate minerals [74,77].
Minerals Crystal structure Morphology Hydration rate Degree of carbonation
C3S Rapid ~20 %
β-C2S Slow ~30 %
γ-C2S Hardly ~50 %
C3S2 No ~40 %
CS No ~30
4
Fig. 3. Schematic representation of carbonation processes of typical calcium silicate minerals [83].
of water, CO2 dissolves and ionizes to form CO2−3 and H . Then, the Ca
+ 2+
that impurities have a significant influence on the formation of car
is released from calcium silicate mineral phase in acidic environment bonate binders.
and diffuses out of the calcium silicate. With the continuous dissolution Saito et al. [87] suggested that the carbonation process of calcium
of Ca2+ and CO2− 3 , supersaturated solution is gradually formed and silicate involved the dissolution of Ca2+ from these particles, leading to
finally results into the precipitation of CaCO3. The dissolved CO2 grad the fast precipitation of Ca(OH)2. Subsequently, Ca(OH)2 reacted with
ually penetrates through the Si-rich area and facilitates the leaching of CO23 to form CaCO3, with calcite being the most dominant polymorph. A
Ca2+. After the leaching of Ca2+, [SiO4] is formed and thereafter leads to small amount of vaterite and aragonite was also detected when using
the formation of orthosilicic acid (Si(OH)4) due to the protonation of some specific carbonation conditions [88]. Apart from crystalline
[SiO4]. Generally, the stability of (Si(OH)4) is low and may rapidly CaCO3, amorphous CaCO3 was also formed during the carbonation of
condense to form silica gel (SiO2). During the carbonation of calcium calcium silicate, which showed lower decomposition temperature
silicate, the mineral composition and carbonation condition may affect (450 ◦ C–625 ◦ C) compared to that of well-crystallized CaCO3, i.e. calcite
the crystal growth of CaCO3 and the polymerization of silica gel [82]. (700 ◦ C–850 ◦ C), aragonite and vaterite (650 ◦ C–700 ◦ C) [78,89–92].
Therefore, carbonate binders consist of different CaCO3 polymers This poorly-crystallized CaCO3 transformed to more stable calcite dur
(calcite, aragonite and vaterite) and silica gel with different degree of ing the subsequent carbonation and hydration [92,93].
polymerization can be generated. Inorganic and organic additives have The morphology, polymorphs and size of CaCO3 changed with time
been proposed as potential regulators to control the composition and during the carbonation of C3S and β-C2S [94]. Wang et al. [82] inves
polymorphous of carbonate binders [84]. tigated the growth of calcite during the carbonation process of C3S and
The carbonation activity of β-C2S is significantly higher than that of proposed the formation mechanism. According to the results of heat
C3S [79]. Jin et al. [85] found that the addition of bacteria could flow, the carbonation process can be separated to three stages. In the
effectively accelerate the carbonation of β-C2S. It did not change the primary heat-releasing stage (i.e., stages I and II), rhombic calcite
crystal form of CaCO3 but had great effects on their morphology and formed from the transformation of amorphous CaCO3, with a slight in
size. The carbonation degree of β-C2S was reduced with the addition of crease in calcite particle sizes. In the stable stage (i.e., stage III), the
NaOH, while a stabilized vaterite phase was formed [85]. Generally, it is particle size of calcite increased significantly. During the carbonation,
considered that impurities can have a significant influence on the the crystal size of calcite increased from 55 to 121 nm. Moreover, the
carbonation of calcium silicate compounds. Mu et al. [86] found that crystallinity of calcite also increased with the carbonation time as its
appropriate content of Вa doping could retard the initial carbonation decomposition temperature increased from 698 ◦ C to 810 ◦ C. They also
reaction but promote the degree of carbonation of γ-C2S. This suggests investigated the development of crystallite size of calcite during the
5
carbonation of β-C2S. Similarly, the carbonation process was divided Moreover, some researchers used coral powder to increase the
into three stages [78]. Different from the carbonation of C3S, the crystal compressive strength and carbonation degree of γ-C2S as its porous
size of calcite sharply increased within the first several minutes of structure could provide more channel for the penetration of CO2.
carbonating β-C2S. Then, poorly crystalline calcite was formed during Carbonated γ-C2S binders can endure the heating when exposed to
the first 12 h and its size increased from 50 nm to about 120 nm after 12 elevated temperature as high as 600 ◦ C, with a notable increase in
h. Besides the calcium silicate minerals, the hydration products of compressive strength observed at 500 ◦ C [110].
Portland cement, can also be carbonated. According to the 29Si MAS Among those calcium silicates, γ-C2S showed the highest carbonation
NMR spectroscopy results, two steps were included during the decom degree, followed by C3S2, CS, β-C2S and C3S [94]. The carbonation
position process of C-S-H gel caused by carbonation [95]. The C-S-H gel mechanisms of non-hydraulic calcium silicates are different from those
was firstly decalcified by removing calcium from the interlayer. With the of hydraulic calcium silicates. During the carbonation of γ-C2S and CS,
decrease of Ca/Si ratio, the calcium was totally removed and convert C- water is absorbed on the surface of these particles and forms a water
S-H to an amorphous silica phase at the second stage [95]. film. Then, CO2 is dissolved in water and forms ions including H+,
For the studies on production of carbonate binders by cement-based HCO−3 , CO2−3 . Meantime, Ca
2+
is formed due to the dissociation of cal
materials, early gaseous CO2 curing for fresh-state cement paste/ cium silicate, and leads to the formation and precipitation of CaCO3 in
mortar/concrete and CO2 curing of hardened concrete products are solution. A Si-rich layer is formed on the particle surface and transforms
widely applied [96,97]. During the process of CO2 curing and/or CO2 into Ca-modified silica gel in the presence of water. Ca-modified silica
treatment, CO2 gas diffuse in the air and dissolve in liquid and finally gel is normally formed around the unreacted CaCO3 particles, while
reacts with the calcium silicate minerals or hydration products within CaCO3 is precipitated in the external space. Finally, Ca-modified silica
cement-based materials to produce carbonate binders, during which the gel gets thick to inhibit the contact between Ca2+ and CO2− 3 , and the
migration, dissolution and reaction processes all control the carbonation reaction rate slows down [111]. C3S, β-C2S and γ-C2S powder showed
rate and efficiency [98]. However, the complex structure and moisture similar carbonation rate when subjected to CO2 curing, while CS showed
distribution within cement-based materials significantly limit the the lowest carbonation rate [90]. Besides, the carbonation process oc
enhancement of carbonation rate and degree, consequently limiting the curs in two stages [39]. Stage 1 is associated with a very rapid rate of
application of these techniques in the production of carbonate binders. carbonation, which corresponds to the phase-boundary controlled pro
cess [112,113]. Stage 2 is characterized by a much slower rate of reac
3.2. Carbonation of non-hydraulic calcium silicate tion, i.e. diffusion controlled reaction [114].
CS with different crystal forms has different carbonation activity, and 3.3. Carbonation of calcium aluminate
α-CS has the highest carbonation activity [99]. High carbonation tem
perature and CO2 pressure can increase the carbonation degree of CS Urbonas et al. [115] found that the different alkali content (1.02 %,
[100] and promote the formation of needle-like aragonite with large 0.56 %) in the same Portland cement had a significant effect on CO2
bending strength [101]. Svensson et al. [102,103] investigated the curing. Carbonation depth, carbonation rate and compressive strength
carbonation of calcium silicate with Ca/Si ratio 1:1. A large amount of are inversely proportional to alkalinity. Moreover, some researcher also
calcite and lower amounts of amorphous CaCO3 were observed. Their found that the carbonation degree increased with the increase of the
study demonstrated the feasibility of using CS-Cement to produce car belite content of Portland cement [116]. Generally, the aluminum phase
bonate binders. Similar to C2S, the incorporation of impurities can also C3A in Portland cement also has carbonation activity, although not as
impact the carbonation process of CS. Zhang et al. [104] proposed a high as that of calcium silicates [75]. The carbonation of C3A is strongly
method to stabilize high-temperature α-CS and studied the effects of affected by the dissolution of C3A at different pH values and the high
sodium doping on the carbonation behavior of α-CS. As sodium doping solubility of aluminum at strongly acidic and basic pH could promote
increased, the early carbonation hardening properties of α-CS were the dissolution and carbonation of C3A [117]. Wang and Chang [76]
slightly lower than those of pure α-CS, but resulted in a significant in found that compared to β-C2S, the carbonation rate of C4AF is higher in
crease in compressive strength and carbonation degree at later stages the initial stage of carbonation (less than 70s). However, as carbonation
[104]. progressed beyond 100 s, the carbonation rate of C4AF decreased
Carbonate binders produced by carbonation of C3S2 are mainly significantly, below that of β-C2S. This was attributed to the decrease in
composed of calcite, vaterite and highly polymerized amorphous silica pH value and Ca leaching. Therefore, it is considered that the carbon
gel, while no presence of aragonite. A rim surrounding calcium silicate ation of C4AF primarily occur in the early stage of carbonation [118].
particles can usually be observed after carbonation, which consists of Aluminum ions re-speciated in the process of carbonation as a result
Ca-modified silica gel or a combination of silica gel and CaCO3 products. of C3A decomposition and partially replace some silicon in the formed
Smigelskyte [105,106] systematically studied the influence of different Q3 and Q4 silicate networks. Prolonged curing time led to increased
factors on the carbonation activity of C3S2. Higher carbonation tem incorporation of Al in silica gel [119]. The main carbonate binders
perature accelerated the formation of carbonate binders during the formed during carbonation of C3A and C4AF are calcite, gibbsite (Al
carbonation of C3S2. The carbonation products in the pastes and mortars (OH)3) and Katoite (3CaO⋅Al2O3⋅6H2O) [76,120]. Besides, traces of
with C3S2 were different. The carbonate binders formed ineRD3 pastes vaterite, aragonite and monocarboaluminate (3CaO⋅Al2O3⋅CaCO3
consisted of three CaCO3 polymorphs including calcite, vaterite, and ⋅11H2O) were also observed in the carbonated C4AF [76].
aragonite, while only calcite was formed in mortar. This difference was
attributed to the presence of the quartz aggregates which promoted the 3.4. Properties and polymorph control of carbonate binders
formation of calcite over other polymorphs.
When the CO2 curing pressure for γ-C2S was increased to 2 MPa, the Within the carbonate binders, CaCO3 was formed during the
compressive strength of formed carbonate binders was 68 MPa and its carbonation process from the reaction between Ca2+ and CO2− 3 through
carbonation degree reached 60 % [107]. Zhao et al. [108] found the two main steps, i.e., nucleation and crystal growth. The crystal growth
addition of chitosan could significantly increase the compressive and was a more complicated step, which was normally initiated with
flexural strength of carbonated γ-C2S due to the formation of coordinate amorphous CaCO3 formation.[143] Thermodynamically unstable amor
covalent bonds by the complexation between calcium ions and the polar phous CaCO3 was then rapidly converted to metastable vaterite or
groups in chitosan. The carbonation reactivity of γ-C2S can also be aragonite and then transformed further to the most stable calcite. The
improved through biomineralization due to the pre-existing calcite transformation of metastable phase to the stable calcite occurred via
formed through biomineralization, acting as nucleation seeds [109]. dissolution and re-crystallization.
6
Considering the various mineral structure of calcium silicate and concentration, temperature and curing time [101,124,125]. Besides, the
other factors on carbonation, the polymorphism of CaCO3 and poly pH of the pore solution affects the formation of crystals [126,127].
merization of silica gel still has no consensus. By using two models of Moreover, the addition of some admixtures may also alter the poly
calcium polymorphs wollastonite (chain-structured) and pseudo morphs. Jin et al. [85] found that the addition of bacterial increased the
wollastonite (ring-structured), Plattenberger et al. [121] reported the degree of carbonation of β-C2S by 16.1 % and the compressive strength
mechanism of CaCO3 formation during the carbonation of calcium sili by 30.1 %. Besides, the size of calcite particles also changed from 3
cate with different crystal structure. As shown in Fig. 4, the release of μm–10 μm cube-like particle to nanoscale particles. As a result, the pore
Ca2+ and Si4+ in the system was different and also played an important structure was greatly improved. The morphology and polymorphs of
role on the morphology of the formed carbonate binders. Generally, the CaCO3 played an important role for the intrinsic properties of carbonate
reaction between wollastonite and CO2(aq) in liquid formed amorohous binders [90]. For example, the stiffnesses of vaterite, aragonite and
silica and CaCO3, while the reaction of CO2 with pseudowollastonite calcite are 39.13GPa, 67GPa, and 72.83 GPa, respectively [128]. It was
produced platelike crystalline calcium silicate phases, along with CaCO3 reported that 20 % to 40 % variation in mechanical performance of
and amorphous silica. carbonate binders generated in a similar carbonation condition may
Crystalline CaCO3 may exist in different polymorphs including happen due to the difference in CaCO3 morphology [90].
spherical vaterite, needle-shaped aragonite and rhomboidal calcite. Mu To control the carbonation products, including the contents of
et al. [77] comparatively studied the carbonation of calcium silicates carbonation products, CaCO3 polymorphs and polymerization degree of
concentrating on the composition and structure of the formed carbonate silica gel, different methods including carbonation condition optimiza
binders. As shown in Fig. 5, unreacted calcium silicate, crystalline tion, addition of chemical agents and biological induced carbonation
CaCO3 and amorphous phase (including amorphous CaCO3 and amor have been proposed and studied [129,130]. During the carbonation of
phous silicate) were the main phases observed in the carbonated calcium calcareous materials or Portland cement-based materials, the relative
silicate minerals. Calcite and aragonite are the preferable polymorphs of humidity [131,132], CO2 concentration [133], carbonation pressure
CaCO3 in the carbonated C3S, γ-C2S, β-C2S, and C3S2, while vaterite only [134] and temperature [124] affect the carbonation rate and degree.
exists in the carbonated CS. The content of these carbonate binders in Therefore, optimization of carbonation condition has been extensively
different systems are also different. Due to the relative low stability of studied for the enhancement of carbonate binders formation to improve
vaterite compared to other polymorphs, the contents of vaterite in the the performance of carbonated concrete products. In recent years,
carbonate binders are generally negligible and it serves as a precursor to bacteria-induced carbonate precipitation has been considered as an
other two polymorphs. environmentally friendly method to accelerate the carbonation re
The morphology evolution of calcite during carbonation has been actions. Some microorganisms can accelerate the precipitation of CaCO3
investigated by studying the carbonation kinetics of calcium silicate in the earth circulation system through a series of physiological activ
minerals [94]. The carbonation time and concentration ratio of CO2− 3 / ities (respiration, metabolism, reproduction, catalysis, etc.), which is a
Ca2+ determined the particle size and morphology of the formed calcite. widely existing complex phenomenon [135,136].
On the other hand, spherical vaterite and needle-shaped aragonite has For the chemical methods, the addition of inorganic and organic
already been successfully synthesized by adding anionic surfactant, and agents can on one hand accelerate the dissolution of calcium silicate
their composition and morphology structure have been studied minerals and CO2 by adjusting pH value and increasing the nucleation
[122,123]. sites, thus enhancing the carbonation rate and formation of carbonate
Many factors affect the formation and polymorphs of CaCO3, and binders [137]. On the other hand, the addition of chemical agents can
different polymorphs can emerge, even when carbonating the same also modify the CaCO3 polymorphs by altering the thermodynamic
calcium silicate and Portland cement [84]. The factors affecting the property and monitoring the transformation of CaCO3 to different
polymorphous of CaCO3 include: 1) Ca/Si molar ratio in calcium sili polymorphous. It was reported that the addition of chelating agent with
cates, 2) initial w/c ratio, 3) CO2 curing conditions such as CO2 low Ca-Ligand stability constant could accelerate the separation of Ca
Fig. 4. Effects of calcium silicate crystal structure on precipitation of carbonation products [121].
7
Fig. 5. Phase assemblage of different calcium silicates carbonated for various durations (a–e), and example of XRD curve fitting by Rietveld refinement (f) [77].
from the complex and transformation of vaterite to calcite [138]. Be mainly amines such as polyacrylic acid (PAA), polyacrylamide (PAM),
sides, formic acid, acetic acid and lactic acid have also been applied to polyvinylalcohol (PVA) and monoethanolamine (MEA) could also
accelerate the Ca leaching from minerals [139]. While, alkaline reagent adsorb on the surface of CaCO3 particles to change the interfacial energy
(e.g., sodium hydroxide (NaOH), ammonium hydroxide (NH4OH)) is and critical nuclear energy, and thus tune the morphology of the newly
introduced to the leachate to increase the pH value and make it more formed CaCO3 [145]. As shown in Fig. 6, the addition of different amines
suitable for CO2 absorption and CaCO3/MgCO3 precipitation [140]. In changed the morphology of the formed CaCO3 crystals [146].
order to increase the fracture toughness of carbonate binders, studies In most cases, only 20–50 % calcium silicates in specimens can be
have been conducted to produce more fibrous aragonite instead of carbonated. Therefore, amorphous silica or silica-rich calcium silicate
calcite in carbonate binders [141]. The divalent cations (such as Mg2+, hydrates (C-S-H) can usually be detected [91]. The silica-rich C-S-H was
Sr2+, Fe2+, Zn2+ and Cu2+) in some inorganic agents can be absorbed by formed due to the incomplete decalcification of original C-S-H from the
calcite and increase the Gibbs free energy, thus lower the stability of normal hydration of cement. It is similar to the original C-S-H gel but
calcite [142]. The addition of MgCl2 agents to facilitate the formation of will eventually transform to silica gel after progressive carbonation ac
aragonite has been extensively investigated [143,144]. Organic agents, cording to SEM-EDX examination [3]. Calcium silicates with high Ca/Si
8
Fig. 6. SEM images of CaCO3 samples induced by 11 selected amines [146].
ratio generates a silica-rich C-S-H gel with higher Ca content after early thick flake to long rod shape and fine-needle shape after 28 days of
carbonation. However, the Q3(OH)/Q4 ratio of the formed carbonate hydration [159]. Plank et al. [75] studied the stability of single phase
binders was nearly the same for all the carbonated-calcium silicate. C3A hydrates under pressurized CO2 condition (7 bar, 20–50 ◦ C). During
Moreover, the calculated Q3/Q4 content ratio indicated that C3S showed carbonation, the ettringite was firstly carbonated to form gypsum,
the highest value, which indicated the lowest polymerization of silica CaCO3 and Al(OH)3, followed by C-A-H gels. After 15 d of CO2 curing,
gel. The similar results were also found in other references [52, 147]. monosulfoaluminate (AFm) started to be carbonated and transform into
γ-C2S can be more easily carbonated compared to β-C2S and the silica- [Ca2Al(OH6)]2(SO4)1-x(CO3)x-LDH. The stability of Katoite was the best
rich phase formed for the former had higher polymerization compared and remained unchanged even after 30 d of CO2 curing.
to that of the latter [148]. Lu et al. [124] found that high temperature
increased the polymerization of silica gel. During further water curing,
3.5. Performance of carbonate binders from the carbonation of
Ca(OH)2 was not detected, which might be due to the reaction between
calcareous materials
Ca(OH)2 and silica gel [149–151]. C-S-H gel also formed during further
hydration after the carbonation, and showed lower polymerization
Carbonate binders produced by the carbonation of calcium silicates
compared to silica gel [152].
and calcium aluminate products usually demonstrates very high
After CO2 curing, the anhydrous minerals within Portland cement
compressive strength within several hours, especially when the pre-
can hydrate and the carbonate binders participate in the hydration re
conditioning process is used. Carbonated low calcium clinker after a
actions during further water curing. The presence of CaCO3 can accel
couple of days of carbonation can even demonstrate compressive
erate the hydration of calcium silicates [153,154]. Some researchers
strength higher than ordinary Portland cement after 28 days of standard
found that the presence of CaCO3 accelerated the transformation of
curing [99].
ettringite to monosulfate [155,156], while some others observed an
The incorporation of SCMs and other admixtures, including lime
opposite phenomena [153]. Monocarboaluminate (3CaO⋅Al2O3⋅Ca
stone [160–162], metakaolin [163], biochar [164,165], pulverized coal
CO3⋅11H2O) (Mc) and hemicarboaluminate (Hc) were detected after
combustion and circulating fluidized bed combustion [166], fly ash
further water curing according to XRD examination [149,151,157] due
[32,167], quartz [168], coral powder calcite seeds [109] and nano-TiO2
to the hydration of C3A in the presence of calcite [158]. Hc was unstable
[169], etc. can provide more space for the growth of carbonate binders
and converted to Mc within 24 h. The morphology of Mc changed from
due to their nucleation effect [170]. Besides, the addition of these
9
admixtures can also introduce more channels for the penetration of CO2, carbonated cement paste were higher than that subjected to conven
such as porous coral powder [171] and rice husk ash [172], or increase tional curing after exposure to high temperature. The high temperature
the CO2 uptake like ground volcanic ash [173]. even improved the compressive strength due to the transformation of
The compressive strength of CO2-cured Portland cement-based less stable polymorphs (vaterite) to stable polymorphs (calcite)
products tends to be proportional to the carbonation degree as shown [110,194,195]. For example, the aragonite in carbonated γ-C2S trans
in Fig. 7. It can be seen that the carbonation degree of Portland cement ferred to calcite at around 500 ◦ C and increased the compressive
samples is less than 40 % and generally increases with CO2 curing time strength [110]. The carbonate and hydrated binders became thermally
and under proper carbonation temperature and relative humidity. stable alite and belite phases when exposed to 1200 ◦ C [194,195]. The
Meanwhile, if Portland cement samples are kept in moist environment Ca leaching resistance of cement paste was also improved by the utili
after CO2 curing, these uncarbonated clinker minerals will hydrate and zation of carbonate binders [196,197] due to the decrease of Ca2+
contribute to the continued strength increase with time. content in CO2-cured cement.
The carbonated Portland cement showed lower porosity due to the The application of carbonate binders enables the use of some waste
continuous formation of CaCO3 and silica gel which have much larger materials in concrete without compromising its strength and durability.
volume compared to raw calcium silicates [149,175–177]. Apart of Chen et al. [198] found that the incorporation of carbonated fly ash in
carbonation, hydration also decreased the porosity of cement [178,179]. cement decreased the resistance of chloride ion penetration of mortar
It was found that the carbonation reaction decreased the percentage of subjected to conventional curing, but CO2 curing mitigated this degra
large capillary pores especially at 0.1 μm–4 μm [180,181], while hy dation by improving the pore structure of mortar [165,199]. Song et al.
dration decreased the amount of capillary pores [182]. The connectivity [200] indicated that the replacement level of fly ash and slag in early
of pores in cement specimens also decreased and the paste with higher CO2-cured cement mortars should not exceed 25 % to ensure a good
w/c ratio of 0.5 showed more pore closure [116,183]. CO2 curing could mechanical and transport properties. Qin eta al. [201] found that CO2
also decrease the porosity of cement paste within the interfacial tran cured cement paste incorporating 20 % of waste autoclaved aerated
sitional zone (ITZ) [184]. The increase of porosity of concrete subjected concrete (WAAC) had comparable strength and chloride penetration to
to longer CO2 curing time was also reported in [185]. The reason behind the pure cement paste. Furthermore, CO2 curing improved the sulfate
this phenomenon is still not clear. Subsequent water curing of carbonate resistance of cement paste incorporating coal gangue, as it led to the
binders could further decrease the porosity of the product [149] and formation of gypsum in place of ettringite [202], which aligns with the
increase the percentage of small pores [141]. results in [203,204].
Concrete subjected to CO2 curing generally showed better durability Jia et al. [205] reported that the formation of carbonate binders,
compared to that with conventional curing. The formation of carbonate especially for CaCO3 enhanced the surface hardness of cement paste
binders could improve the resistance to the chloride-induced corrosion compared to the internal layer [206,207]. Subsequent lime water curing
of concrete due to the densified carbonate-rich surface layer [186,187]. and the incorporation of SCMs further decreased the permeability and
Besides, the pH in the core of concrete subjected to ambient CO2 pres chloride migration coefficient [55,157]. Xu et al. [208] investigated the
sure was high, which is beneficial in protecting the steel in reinforced coupled effect of carbonation and bio-deposition on the properties of
concrete [187,188]. Zhang et al. [189] suggested that CO2 curing could concrete and found that concrete subjected to these two treatments
potentially be applied to reinforced concrete without the risk of showed lower water absorption and water permeability compared to
carbonation-induced corrosion as the pH reduction resulted from CO2 that subjected to each treatment separately.
curing could be restored through post hydration. Due to the reduction of
calcium hydroxide content and the densification of the microstructure, 4. Carbonate binders from magnesium-based materials
the use of formation of carbonate binders decreased the alkali-silicate
reaction-induced expansion of waste glass-blended cement by up to MgO cement can be easily carbonated to produce carbonated MgO
85 % [190], increased the properties after natural and accelerated cement (CMC). De Silva et al. [209] found that the interlocking network
weathering [191,192] and improved the resistance to low temperature structure formed by interconnected and well-developed crystals (such as
sulfate attack [193]. The residual mechanical properties of the Nesquehonite) controlled the overall performance of CMC. Research on
the factors that affected CMC system started from the influence of water
and cement content on compressive strength [210]. Vandeperre et al.
[50] found that the reactive MgO cement (RMC) mixed with 10 %
cement showed much higher compressive strength than the pure CMC
sample. Subsequently, a series of studies on other factors such as the CO2
concentration (environment and 20 % CO2 concentration) [211], type
and saturation level of aggregates [210], and particle size distribution
[212] were published. With the improvement of the engineering appli
cation requirements, researchers began to pay more attention to the
durability of the CMC system, and suggested the use of hydrochloric acid
and magnesium sulfate solution to ensure a better durability [213].
SCMs were also used in CMC system. It was found that the accelerated
carbonation of CMC-PC mixed with ground granulated blast furnace slag
would lead to the formation of nesquehonite, calcite and aragonite
[51,214,215]. The formation of magnesium silicate hydrate (M-S-H) and
hydrotalcite in the presence of fly ash was also reported [216,217].
4.1. Carbonation of magnesium-based materials
The magnesium sources with carbonation potential can be divided

into three categories: (1) magnesium oxide-based binders (such as the
Mg oxychloride cements (MOC), Mg phosphate cements (MPC) and Mg
Fig. 7. Compressive strength as a function of carbonation degree. oxysulfate cements (MOS)); (2) magnesium silicate-based rocks (such as
(Data from ref. 43, 44, 147, 174). Olivine, Serpentine and Talcum powder); (3) other magnesium sources
10
such as industrial waste brine. Their chemical compositions and main xMgCO3⋅yMg(OH)2⋅zH2O. With the change of the composition of raw
reaction products are shown in Table 3. Magnesium oxide-based mate materials in the system, the proportion of different HMCs will also
rials show high CO2 absorption ability (1.09 metric tons per metric ton change [213].
of MgO [218]). The main reaction process involves the formation of The microscopic morphology of the most HMCs is shown in Fig. 8.
brucite after hydration and the subsequent reaction with CO2 to form Magnesite, hydragnesite and a small part of dypingite are found in the
various hydrated magnesium carbonate products. The mineral carbon carbonation system of magnesium oxide-based materials [229–231].
ation of magnesium silicate-based rocks shows great potential for CO2 Magnesite tends to cover the surface of carbonation area, resulting in the
sequestration because the available olivine resources are abundant. It is densification of microstructure. For magnesium silicate-based materials
estimated that the olivine resources are sufficient to store all anthro such as talc and serpentine, nesquehonite with a needle-like morphology
pogenic CO2 emissions in the next 1000 years to produce carbonate and interlaced network are the main carbonation products. Although the
binders [219]. In many areas where limestone and clay minerals are mohs hardness of nesquehonite is close to that of brucite (~2.5), the
scarce, magnesium silicate-based minerals are an excellent choice for nesquehonite system is more compact due to its monolithic nature
sustainable binder production. However, it should be noted that high [224]. CaCO3 is another main carbonation product as CMC and PC are
CO2 pressure and temperature is generally required for the carbonation usually mixed in the application situation. Different from the carbonated
of olivine according to the carbonation kinetics [219]. In addition, other PC system, in the carbonated CMC-PC system, the magnesium ions will
magnesium sources, such as the industrial waste brine [220,221], can affect the composition of CaCO3, leading to the formation of magnesium
provide concentrated magnesium solution for CO2 sequestration. substituted CaCO3 and aragonite [51,214]. Recently, Li et al. [232]
The carbonation of magnesium cement includes three stages: hy studied the effects of the incorporation of lime on the formed carbonate
dration of activated magnesia materials, dissolution of CO2, and the binders of carbonated RMC. The incorporation of lime increased the CO2
carbonation reactions. For instance, in the case of magnesium oxide, adsorption capacity of blended RMC due to the increased formation of
magnesium oxide reacts with water during the first stage to form mag calcite. Moreover, the content of nesquehonite was increased due to the
nesium hydroxide clusters on its surface. The formation of brucite enhanced carbonation of Mg(OH)2. With the addition of CaCO3 poly
continuously consumes the free magnesium ion in the solution, thus morphs from limestone, new carbonation products of amorphous phases
further promoting the dissolution of active magnesium mineral. The with a hydromagnesite-like and fused structure were also observed
precipitated brucite layer will separate the reactive surface from the [233].
reactive component, thus limiting the hydration reaction [224]. This Compared to calcareous materials, the carbonate binders produced
part of reaction is controlled by the diffusion process. However, with the from carbonation of magnesia phases exhibit greater complexity. The
continuous hydration reaction, the brucite layer begins to crack due to various sources of magnesium phases results in different carbonation
the volume expansion, resulting in the exposure of the fresh and reactivities and other properties. Therefore, studies on regulating the
unreacted MgO surface [225]. Similar to carbonation of calcium silicate carbonate binders and improving mechanical properties of CMC has
phases, during the carbonation of magnesium materials, the dissolution been conducted [232]. However, further researches are still needed to
of CO2 is an indispensable process, in which gaseous CO2 is converted classify the magnesia sources and improve the carbonation degree and
into CO2 (aq), carbonate, bicarbonate and hydrogen ions in the liquid performance of CMC.
phase. The concentration of these ions is mainly determined by the pH
value of the solution and also affected by the temperature. As the 4.3. Mechanical properties and durability of the carbonate binders
dissolution process of CO2 proceeds, the carbonate ions will react with
magnesium hydroxide or magnesium silicates to produce various hy Compared with the equivalent calcium-based system, magnesium-
drated magnesium carbonate products (HMCs). In recent studies based carbonate binders have higher compressive strength and stron
[226,227], microbial carbonation process was proposed to accelerate ger binding ability [235], making the strength of CMC develop very fast
the dissolution of CO2 into CO2−3 ions in the pore solution to facilitate the during carbonation. The carbonation reaction of CMC is an expansion
carbonation of magnesium cement and formation of HMCs. Moreover, it process, which leads to the increase of solid volume and the decrease of
was also reported that the implementation of a hydration agent and high porosity. Besides, the formation of various forms of HMCs is conducive
temperature pre-curing increased the content of hydration products to the evolution of an interlocking network structure. The compressive
(mainly brucite) and further enhanced the carbonation degree of RMC- strength of CMC is gradually increased with the formation of HMCs such
based concrete [228]. The classification and composition of different as nesquehonite, artinite, hydrogenesite and dypingite. The increase of
HMCs can be found in Section 4.2. pristine nesquehonite is beneficial to the formation of starlike clusters,
which leads to the increase of the density and development of inter
4.2. Carbonate binders from the carbonation of magnesium materials locked network structure [209]. It has special adaptability in crack
healing, so carbonated magnesia materials can be used in the production
As shown in Table 3, the carbonation products of CMC include a of autogenic healing engineered cementitious composites [236]. When
series of HMCs, which can be represented by a general formula 25 % magnesium oxide is added to wollastonite and slag composites, the
compressive strength increased by 44 % and 126 % respectively [237].
Table 3 However, as the carbonation time prolonged, the strength of CMC
Various magnesium sources and the main carbonation products. slightly decreased due to cracks originated from the uneven distribution
Reactants Chemical Main carbonation products References and expansion of HMCs [238].
(Mg sources) compositions CMC shows excellent corrosion resistance to hydrochloric acid and
Magnesite (MgCO3),
magnesium sulfate [213]. Most carbonate binders such as bischofite,
Magnesium hydrotalcite and calcite, are stable under chloride attack [239]. Fig. 9
MgO Hydromagnesite [222,223]
oxide
(Mg5(CO3)4(OH)2⋅4H2O) shows SEM images of CMC samples before and after 12 weeks of expo
Olivine Mg2SiO4 Nesquehonite (MgCO3⋅3H2O) [221] sure to NaCl and cyclic wet/dry conditions [239]. It can be seen that
Talcum Magnesite (MgCO3),
Mg3Si4O11(OH)2 [224] CMC samples retain a significant portion of the dense network composed
powder Nesquehonite(MgCO3⋅3H2O)
Serpentine Mg3Si2O5(OH)4 Nesquehonite (MgCO3⋅3H2O) [221,224] of rosette-like hydromagnesite and needle-like nesquehonite after wet
Industrial and dry cycles. The addition of an appropriate amount of fly ash can
waste MgCl2 Magnesite (MgCO3) [220,221] improve the chloride ion resistance of CMC, as it does not alter the dense
brines network formed by HMCs and reduces the content of permeable pores.
Although a decrease in compactness was found in samples mixed with
11
Fig. 8. SEM images of different carbonation products from magnesia system (a) magnesite [230], (b) nesquehonite [234], (c) hydromagnesite [229] and (d)
dypingite [231].
Fig. 9. SEM images before exposure to cyclic wet/dry conditions (a) 40 %RMC, (b) 20%RMC +20%FA and (c) 20%RMC + 20%GGBS, and after exposure (d) 40 %
RMC, (e) 20%RMC +20%FA and (f) 20%RMC + 20%GGBS [239].
slag, a large amount of needle-like nesquehonite and hydrotalcite with nesquehonite improved the strength, water stability and enhanced
excellent chloride binding capacity could still be observed. resistance to dry-wet cycles and freeze-thaw cycles of carbonate binders.
Wang et al. [240] studied the microstructure and mechanical prop The phase transition from dypingite and nesquehonite to hydro
erties of carbonated MgO-FA solidified sludge and found that the skel magnesite happened during the continuous water curing and dry-wet
eton formed by elongated prismatic hydromagnesite, pore filling and cycle experiments. Although no obvious phase transition was detected
particle cementing effects due to the formation of dypingite and during the freeze-thaw cycle, the content of macropores with a radius
12
greater than 10 μm increased significantly. In addition to permeability, Besides, MS exhibits pretty good CO2 sequestration efficiency due to its
proper addition of magnesium oxide was also found to increase the CO2 high free MgO and CaO contents.
absorption capacity of calcium oxide-based materials at high tempera
tures. After 50 carbonation and decarbonation cycles at 758 ◦ C, the CO2 5.1. Fly ash
absorption capacity of the CaO-MgO mixture prepared by this method
was 53 wt% higher than the control group [241]. The magnesium added FA is a non-hydraulic material, and its carbonation activity is not as
in alkali-activated slag paste can form a stable amorphous CaCO3 phase good as cement clinker. Several key factors, such as chemical compo
containing magnesium, which can prevent the removal of additional sitions, particles sizes, temperature, CO2 concentration, and pressure
calcium from C-A-S-H gel, thus improving the carbonation resistance of will all affect the carbonation process and CO2 fixation efficiency of FA
the materials [242]. This may be of great significance for their use in [251]. FA can be effectively used to produce carbonate binders when the
extreme corrosive environments involving the use of CO2 for oil recov calcium content is large. The carbonatable minerals in FA are mainly
ery and geological reserves. Generally, a relatively high temperature is lime and portlandite, leading to the formation of CaCO3 composed of
needed for the carbonation of magnesium phases, which limits the ap different polymorphous [245]. Many researchers conducted aqueous/
plications of magnesia-based carbonate binders. wet carbonation under elevated temperature to enhance the carbonation
capacity and efficiency of FA [252,253]. Fig. 10 depicts the compressive
5. Carbonate binders from industrial by-products and cement strength evolution of cement-FA mortar with standard and CO2 curing
waste [251]. As can be seen, the addition of FA decreased the compressive
strength at early age, and the synergy of carbonation treatment and CO2
Besides to the pure calcium silicate compounds and Portland/ curing effectively mitigated this degradation. It was considered that the
magnesia cement, some by-products such as blast furnace slag (BFS), carbonation delayed the strength development brought by pozzolanic
steel slag (SS), magnesium slag (MS), fly ash (FA), cement kiln dust effect due to the heavily consumption of Al2O3 and decreased specific
(CKD) and also cement waste which are rich in alkaline earth metals (e. area of FA. It has been confirmed that FA from coal fired power plant can
g. CaO, and MgO) could also react with CO2 to produce carbonate be applied for CO2 capture and the results showed that the carbonated
binders [97,243]. Moreover, the solid waste from demolished concrete FA was feasible to be used as a mineral admixture for cement concrete
structure can be recycled as carbonate binders [98]. However, industrial [254]. Chen et al. [255] mixed carbonated FA and cement to develop
by-products and cement waste have complicated mineral compositions, carbonate binders. Up to 30 % carbonated FA was incorporated to
and their carbonation capacities are lower than Portland cement. The replace cement in mortar. After 12 h of standard curing, the specimens
composition and structure of carbonate binders produced by industrial were stored in a carbonation reactor for 8, 16, and 24 h. The results
by-products and cement waste from various source can differ with each showed that the carbonated FA decreased the hydration heat of cement
other. These make it difficult to utilize carbonate binders produced from mortar and accelerated the hydration rate at early age due to the micron-
industrial by-products and cement waste for large-scale application. grade carbonates generated on the surface of FA. By using ultraviolet
The CO2 uptake capacities of industrial by-products depends greatly pretreatment, it was also found that the CO2 uptake and properties of FA
on the CaO and MgO content. Table 4 compares the amount of generated cement were significantly enhanced with low CO2 concentration due to
(output) and the theoretical maximum CO2 uptake of different industrial the decrease of water content to unlock the channel for the entry of gas
by-products. The output of industrial by-products, in a descending order, [256].
are FA, CKD, BFS, basic‑oxygen furnace slag (BOFS), electric-arc furnace The permeability of concrete to chloride ions could be significantly
slag (EAFS), ladle furnace slag (LFS), and MS. It can be noted that the increased when using carbonated FA, which was mainly caused by the
theoretical maximum CO2 uptake of FA significantly varied within a fully consumption of portlandite and presence of carbonates. Su et al.
wide range between 3.93 % and 42.31 %. This is because FA has huge [257] investigated the freeze-thaw resistance and sulfate attack resis
differences in the active CaO content. The chemical composition of CKD tance of cement-FA mortar subjected to carbonation. The results
is similar to that of cement clinker, but the CaO content is lower. As a demonstrated that synergistic of carbonation treatment of FA particles
result, the CO2 uptake capacity of CKD is quite low, between 28.28 % and CO2 curing of mortar significantly reduced the compressive strength
and 39.10 %. Steel slag is one of the industrial by-products from steel loss in freeze–thaw and sulfate attack due to the two aspects: (1) the pore
manufacturing, which accounts for 15 to 20 wt% of crude steel pro structure got improved after carbonation and the water penetration
duction [11,244]. It can be divided into three categories according to the decreased; (2) carbonation process consumed free CaO and Ca(OH)2 to
main production processes used in the production of steel (e.g. BOFS, reduce the expansion caused by the delayed hydration and sulfate
EAFS, and LFS). BOFS accounts for the majority of steel slag output. The attack.
CaO content of BOFS is slightly higher than that of EAFS, so BOFS could
sequester more CO2. LFS contain less Fe and more Ca, so the theoretical
maximum CO2 uptake of LFS is higher than that of BOFS and EAFS.
Table 4
Main industrial by-products and their theoretical maximum CO2 uptake.
Industrial by- Output (Mt/ Alkaline earth Carbonatable minerals Theoretical maximum CO2 uptake References
product y) metals content (%)a
(%)
CaO MgO
FA 750–1000 5–40 0–10 Lime (CaO), portlandite (Ca(OH)2) 3.93–42.31 [245]

CKD 670 34–46 1–3 Lime, portlandite, calcium silicates 28.28–39.10 [246]
BFS 390 29–50 0–21 Gehlenite (Ca2Al2SiO7), akermanite (Ca2MgSi2O7) 22.77–62.16 [247]
Belite (Ca2SiO4), alite (Ca3SiO5), portlandite, lime, periclase
BOFS 140 35–60 2–10 29.66–58.01 [248]
(MgO)
EAFS 70 25–47 3–13 Belite, alite, lime, periclase 22.89–51.08 [249]
LFS 30 42–57 4–12 Belite, lime, periclase, merwinite (Ca3MgSi2O8) 37.33–57.84 [9]
MS 8 42–54 4–17 Belite, alite, lime, periclase 38.16–61.55 [250]
a
Note: The theoretical maximum CO2 uptake is determined according to the content of CaO and MgO contained in the industrial by-products.
13
Fig. 10. Compressive strength of standard and CO2-cured cement-fly ash mortar [251].
5.2. Cement kiln dust changes from metastable to stable carbonates leads to needle-like pro
trusions penetrating throughout the glassy material. This process is very
Cement kiln dust (CKD) is generated inside the cement kiln, where unique because it creates a clinker material with advanced carbonation
the temperature ranges between 800 ◦ C and 1000 ◦ C, at levels of 10 to before hydration. Matalkah et al. [260] adopted similar method to
15 wt% of the clinker [258]. High free lime content in CKD endorses it prepare MCCA powder and added sodium hydroxide and sodium silicate
certain carbonation capability. Alimi et al. [246] used CKD as a partial to mold the geopolymer concrete specimens.
replacement of cement (0–60 %) in mortar specimens subjected to CO2
curing. The results showed that 4 h of CO2 curing could attain about 80
5.4. Steel slag
% of total CO2 uptake with 12 h CO2 curing. According to the obtained
results [246], pH values of the mixtures containing CKD were within a
Steel slag is a by-product produced during the steel manufacturing
narrow range of 13.05 and 13.32, and slightly increased with CKD
process and can be divided into three categories according to the pro
content. Thus, CKD served as a hyper-alkaline constituent that offered a
duction processes of steel, e.g. basic‑oxygen furnace (BOF), electric-arc
viable remedy to aerated CO2 curing induced dealkalization of concrete.
furnace (EAF), and ladle furnace (LF) slags. The main minerals of steel
Sharma et al. [37] investigated the effect of aerated CO2 curing on
slag include tricalcium silicate (C3S), dicalcium silicate (C2S), tetra-
mortar made by using CKD as partial replacement of cement. The mortar
calcium aluminoferrite (C4AF), dicalcium ferrite (C2F), glassy calcium
exhibited better 3 d compressive strength, exceeding 120 % of the
aluminosilicate phases and RO phases (solid solution containing mag
strength of samples subjected to water curing. This indicated that
nesium, iron, and manganese oxides) [11,261,262]. However, the low
carbonation process may promote hydration process. The fine particle
content of C3S and high content of C2S phase result in poor hydraulic
size of CKD and the presence of alkali may also contribute to the higher
property of steel slag. The components of steel slag such as C2S, C3S and
strength. Depending on CKD replacement level, mixtures with w/b ratio
alkaline oxides containing calcium and magnesium can react with CO2
of 0.5 sequestrated 40–170 % more CO2 than that with lower w/b ratio,
to form carbonate binders with better volume stability [263,264]. Ma
suggesting that higher w/b ratio was favorable to maximize CO2 uptake.
et al. [265] studied the effects of concomitant elements in steel slag
including iron/silicon/magnesium/aluminum on carbonation of cal
5.3. Blast furnace slag cium phases. It was found that the occurrence of Fe2O3, Fe3O4, MgO and
Al2O3 could provide more surface area for precipitation of carbonate
Several researches have studied the carbonation efficiency of blast binders and avoiding in-situ aggregation. Thereafter, the carbonation
furnace slag, revealing that approximately 30 % of calcium in slag could degree was increased. Generally, RO phases account for around 10-15
be converted into carbonates [245]. However, due to the formation of wt% of steel slags and always result in its poor volume stability. By dry
Ca-depleted silicate rim on the surface of particles, the diffusion of Ca2+ carbonation, it was found that leaching of Mg was accelerated and
and CO2−3 can be hindered during direct carbonation process. Therefore, further enhanced the reaction rate of steel slag and the performance of
indirect carbonation by incorporating different ammonium salts to leach steel slag-cement mixtures [266]. The wet carbonation technique has
blast furnace slag have been proposed [259]. Marple et al. [244] com also been used to improve the volume stability of RO phases in steel slag
bined mechanical activation and alkali activation for a mixture of 90 wt [267]. The formation of CaCO3, can further improve the microstructure
% granulated blast furnace slag and 10 wt% Na2CO3. The mixture was through its filling effect [268–270]. Thus, accelerated carbonation of
milled in a rotary ball mill in a CO2 rich atmosphere for 2 h. The steel slag is an environmentally friendly way to eliminate free CaO and
resulting powder was named as a mechanical alkali-activated (MCCA) MgO, effectively inhibit the leaching out of heavy metals [271], and
powder. The process breaks through the diffusion limitation of carbon sequestrate CO2 [272].
ation and the milling continually creates unreacted surfaces for Liu et al. [273] developed a high performance carbonatable concrete
carbonation to occur. The metastable carbonate binders resulting from with 90 % closely-packed steel slag. The samples had high flowability
the MCAA process, i.e., bicarbonates, carbonates incorporated within and the compressive strength reached 104.9 MPa and 173.7 MPa,
the aluminosilicate network, and amorphous CaCO3 gradually become respectively, after 12 h and 7 days of CO2 curing. The excellent me
hydraulic phases. After hydration, the CaCO3 phases of calcite and chanical property of carbonated steel slag concrete is resulting from the
aragonite, and hydrated carbonate phase gaylussite form. These radical densification effect of carbonate binders and also the pre-designed
14
closely-packed skeleton. Mahoutian et al. [269] prepared cementing 5.6. Recycled concrete fines
binders using two typical ladle slag through CO2 curing. They found that
the slag containing higher silica (C3S and C2S) showed higher Recycled concrete fines (RCFs) are generated during the production
compressive strength and CO2 uptake. Generally, the carbonate binders of recycled aggregate. Its higher water demand results in lower work
formed in carbonation of steel slag consist of calcite and amorphous ability [279,280] and mechanical properties [281,282]. RCFs consist
silica due to the high percentage of C2S in most steel slag. However, it mainly of C-S-H and Ca(OH)2 and can be carbonated and converted to
was found that with the addition of amino acids, vaterite was also CaCO3 and silica gel [57]. Conventional solid-gas carbonation method
formed and the carbonation degree was enhanced as shown in Fig. 11 (dry carbonation) has slow carbonation rate and limited carbonation
[274]. Therefore, it is an efficient way to enhance the properties of degree [283]. Recently, wet carbonation has been developed to accel
cement mixed with carbonated steel slag. erate the carbonation of RCFs [57,284]. Zajac et al. [285] proved that
However, the slag containing high lime and alumina showed no the wet carbonation of RCFs was a dissolution (diffusion)-precipitation-
carbonation reactivity in spite of its high CaO content. In other words, controlled process, including (1) dissolution of CO2 in water; (2) disso
the CO2 uptake was related to the reactive CaO content rather than total lution of Ca-bearing phases in water; (3) precipitation of CaCO3 and
CaO content [275]. The compressive strength of carbonated ladle slag alumina-silica gel; and (4) the transport of species from the dissolution
increased continuously during subsequent hydration period [276]. Wei surface to the precipitation surface. A higher surface area of the RCF
et al. [277] studied the effects of desulphurisation gypsum on the hy particles is exposed to the dissolved CO2 in the aqueous suspension
dration and carbonation reactivity of steel slag with mass ratio 16:1 [286], which further promotes the dissolution of calcium [287]. Ho et al.
(steel slag to gypsum), and found that the samples subjected to 1 d of [288] proved the feasibility of using atmospheric pressure and CO2
hydration then followed by 2 d of carbonation showed the highest concentrations of 14 % to wet carbonate RCFs.
compressive strength of 57.56 MPa. The SEM-EDS analysis also depicted Some researchers [22,289–292] have applied carbonated RCFs as
that the main carbonatable minerals were C2S and C3S, and the CaCO3 SCMs to replace cement. Silica gel can react with Ca(OH)2 in a pozzo
particles formed during carbonation can fill the internal voids. With the lanic reaction. Zajac et al. [57] proposed a one-step wet carbonation
addition of desulphurisation gypsum and hydration curing, needle-like method by NaOH solution to produce carbonated recycled cement paste
AFt and amorphous C–S–H gel form. fine as a SCMs. The formed carbonate binders are reported to be a
mixture of calcite, alumina-silica gel and alkalis. By using this method,
Lu et al. [22] found that the carbonated RCFs consist mainly of calcite
5.5. Magnesium slag and silica gel, with calcite accounting for approximately 55.2 %. The
compressive strength at 7d and 28d of cement paste mixed with 20 %
Magnesium slag is a kind of by-product of the magnesium industry. dry carbonated RCFs was 21.9 % and 12.1 % higher than that of ordi
Its application is very limited due to its poor hydration reactivity and nary Portland cement paste. Recently, Fang et al. [284,293] developed a
high content of free MgO and CaO [278]. However, its high CaO and two-step wet carbonation technique to valorize old hydrated cement
MgO contents will be suitable for CO2 treatment. pastes to produce calcite and alumina-silica gel, separated by reusing a
The carbonated magnesium slag paste showed a stable volume Na2CO3 solution. Ouyang et al. [294] reported that 40 % carbonated
whereas the magnesium slag paste without CO2 activation was RCFs as cement replacement resulted in better strength development.
completely disintegrated due to the excessive expansion as a result of the Due to the strong affinity for H2O of the silica gel on the surface of CRP,
hydration of lime and/or periclase. According to the pore structure of the cement paste with carbonated RCFs showed a higher flowability
magnesium slag paste, after 1 d and 14 d of CO2 carbonation, the total despite the larger particle size of carbonated RCFs and lower surface
pore volume in the carbonated magnesium slag paste (0.016 cm3/g) was area than the uncarbonated ones. The roles of RCFs in the blended
much smaller than that in the samples before carbonation (0.115 cm3/g) cement include: (1) calcite can react with aluminates in cement to form
[278]. The formation of CaCO3, mainly calcite and vaterite, led to an calcium carbon aluminate, which prevents ettringite reacting with C3A
improved matrix with dense microstructure, and increased compressive and C4AF and ensure the stable presence of ettringite [22]; (2) calcite
strength. Lei et al. [250] proposed a CO2 activated aerated concrete provides a large number of nucleation sites for C-S-H and promotes their
(CAAC) with varying densities (400, 600, 800 kg/m3) with magnesium precipitation [22,294,295]; (3) calcite fills the intra-particle voids be
slag as the primary binders which achieved a compressive strength and tween cement particles and increases the bulk density of the matrix
carbonation degree around 7 MPa and 55 %, respectively. The superior [158,295]; (4) silica gel has good pozzolanic activity and can react with
mechanical properties were resulted from the evolution of microstruc Ca(OH)2 to produce more C-S-H [22,58,294]. Zajac et al. [58] suggested
tural morphology and low porosity as shown in Fig. 12.
Fig. 11. Stabilization mechanism of vaterite under the action of amino acids [274].
15
Fig. 12. 3D void connectivity images of CO2 activated aerated concrete [250].
that the high volcanic activity of silica gel was the dominant factor humidity larger than 95 %,) which had compressive strength and other
influencing cement hydration. properties of concrete blocks that meet the requirements of the relevant
In addition to the direct carbonation treatment, some researchers national standards as shown in Fig. 13 [60]. It is estimated that it will
calcined the RCFs to form regenerated cementitious materials for CO2 consume about 26,000 t of CO2 and generate 3.79 million Kw⋅h elec
curing. β-C2S and CaO formed after calcination [296] showed high tricity from saved steam annually. In this project, the carbonation de
carbonation reactivity. When exposed to a CO2-rich environment, gree of the carbonatable materials in concrete brick can reach 50 %. The
CaCO3 and silica gel were generated [297,298], and high compressive carbon tax in the trading market of China is around 76 yuan/ton, which
strength was obtained. The carbonated RCM mortar achieved a 75.2 % the highest carbon tax in a recent auction has reacted 485 yuan/ton.
reduction in global warming potential (GWP) compared to Portland Considering the price of Portland cement as 280 yuan/ton, the cost to
cement mortar [299]. Some researchers used high temperatures to produce one concrete brick can be decreased from 0.21 yuan (steam
calcine RCFs as high temperature has a positive effect on the improve cured bricks) to 0.08 yuan (carbon tax 76 yuan) and − 0.09 yuan (carbon
ment of the carbonation reactivity of RCM. While other researchers used tax 485 yuan). However, cause the carbona tax in Europe is almost 800
low temperatures and obtained mortars with compressive strength of 50 yuan/ton, the cost to produce concrete brick is − 0.23 yuan. At present,
MPa after 2 h of CO2 curing [300]. the carbonated concrete bricks have been applied in the constructions of
pavement, slope protection and building wall.
6. Demonstration and applications
6.2. CO2-SUICOM technology
The carbonate binders have been studied for many years, but their
commercial application is limited due to the high cost of CO2 capture KAJIMA CORPORATION in Japan developed a low-carbon concrete
and purification. In recent years, several companies have developed named CO2-SUICOM (CO2 Storage under Infrastructure by Concrete
proprietary carbonate binder, products or processes to utilize CO2 curing Materials) with three features: (1) γ-C2S was utilized instead of cement
technologies. Moreover, in order to lower the cost of CO2 capture, the as this material has a very low level of CO2 emission and can react with
utilization of industrial waste gas with low CO2 concentration, high CO2; (2) CO2 curing technique was used to cure this concrete; (3) in
relative humidity and large impurity contents in production of carbon dustry by-product such as coal ash was incorporated to replace cement,
ate binders have been studied. as shown in Fig. 14. The compressive strength of this concrete could
reach 21.6 MPa after CO2 curing. The CO2 amount fixed by concrete was
6.1. CJS technology 100 kg/m3 and the CO2 emission was − 13.9 kg/m3 including that
originating from materials [62]. Researchers in the University of Tokyo
In 2003, McGil University and CJS Technology Inc. successfully ac also proposed a new CaCO3 concrete comprising a binder of CaCO3 and
quired a Canadian NSERC GHGM project on “CO2 Sequestration in aggregate from concrete waste to reduce CO2 emission and recycle
Concrete through CO2 Curing”. After that, Shi and his colleagues firstly construction waste [302], as presented in Fig. 15. The mold is filled with
put forward the theory of “moisture regulation-gas migration-carbon carbonated hardened cement powder. When the solution can no longer
ation reaction” and developed the pre-curing technology, which signif pass through the mold, the hardened concrete is removed from the mold.
icantly increased the carbonation rate and degree of cement-based The compressive strength of this concrete was 8.6 MPa with a porosity of
materials and made the large scale production of CO2-cured concrete 46 %. The major binding phase of CaCO3 was needle-like aragonite.
products possible [31,301]. In 2021, they established the world's first
commercial scale CO2 curing production line using CO2 from cement
kiln exhaust gas (15–20 % volume concentration of CO2, relative
16
Fig. 13. Production of CO2-cured concrete blocks using CJS technology [60].
Fig. 14. CO2-SUICOM concept [62].
Fig. 15. Schematic illustration of the production process of CaCO3 concrete [302].
6.3. Solidia technologies to the lower calcination temperature, the production of CSC clinker reduces
the fossil fuel consumption by as much as 30 % [303]. Refer to the total CO2
Solidia Technologies proposed a low-carbon calcium silicate-based emission, CSC clinker production offers a reduction of CO2 emission by
cement (CSC) to replace Portland cement for CO2 curing in 2011 [21]. Its about 30 % compared to cement industry [21]. Formed CSC-based concrete
primary constituents were CaSiO3 (wollastonite) and Ca3Si2O7 (rankinite) will be exposed to water and gaseous CO2 for CO2 curing. Thin concrete
along with complex CaAlSiO-based phases (melilite), which showed much products such as roof tiles (~10 mm thick) can be cured in less than 6 h.
lower lime content compared to Portland cement. The total lime content of Larger concrete parts (~250 mm thick) can be cured within 24 h. During
CSC clinker is in the range of 45–50 %, which is 30 % less than that required the CO2 curing process, up to 300 kg of CO2 per ton of CSC can be absorbed
for PC. As a result, the total theoretical enthalpy of formation of CSC clinker [304]. It was reported that the Solidia cement had lower thermal conduc
is about 1.05 GJ/t, which is almost 40 % lower than that of PC clinker. Due tivity, and higher fire resistance.
17
6.4. Carbstone (2) Carbonate binders and CO2 curing technique are extensively
investigated in recent years and most research focused on the
In collaboration between VITO and the Walloon CTP of Belgium, early age performance. Thus, the durability performance of car
Carbstone Innovation technology was patented and the products named bonate binders needs further study, such as high temperature
Carbinox® was introduced, designed to carbonate steel slag to seques resistance, chloride permeability, wet-dry cycle resistance,
trate CO2 and produce different low carbon materials including floor carbonation resistance, and freeze-thawing resistance of mate
tiles, roofing tiles, clinkers and building blocks [305]. It uses 100 % steel rials incorporating carbonate binder.
slags to form different shape with required compressive strength and (3) As regard to the carbonate binders, the previous studies mainly
other properties. Autoclave carbonation is applied in this technology focused on carbonation products of the pure Portland cement.
and the formed CaCO3 within the porous stones can assure that the The studies about the properties and microstructure of carbonate
performance of carbonated concrete products have the same charac binders produced by carbonation of different SCMs or blended
teristics as classic brick products. materials are limited. Therefore, the composition and structure of
Besides to the calcium phase materials, carbonate binders produced carbonate binders from carbonated Portland cement-SCMs
by magnesium phase also has some applications. A Chinese company blended materials should be further studied.
called Doric and China Building Materials Academy Co., Ltd. have also (4) Many additives were added in cementitious material to promote
been granted patents about the production of magnesium carbonate carbonation. But the improvement is limited and the carbonation
products by carbonation [306]. degree was lower than 50 %. Therefore, there is an urgent need to
identify or develop some additives to further increase the
7. Conclusions and perspectives carbonation degree of carbonatable binders.
(5) Even though the CO2 curing of cementitious materials decreases
7.1. Conclusions the CO2 emission, it may increase the energy consumption if pure
CO2 is utilized. Thus, the carbon footprint and life cycle assess
This paper reviews and provides insight into how carbonate binders ment of the CO2 curing technique should be further studied.
and carbonation techniques have been developed, analyzed and used
during the past decades. The following conclusions can be drawn from CRediT authorship contribution statement
this review:
Xiang Hu: Conceptualization, Investigation, Visualization, Formal
(1) The first investigation of carbonate binders in cementitious ma analysis, Data curation, Writing- Original draft preparation, Writing –
terials by CO2 curing or treatment was initiated in 1970s. The Review & Editing.
application of pre-conditioning technology accelerates the Pingping He: Validation, Conceptualization, Methodology, Investi
application of carbonate binders in construction materials. gation, Data curation, Formal analysis, Review & Editing.
(2) The hydraulic and non-hydraulic calcium silicates are the main Caijun Shi: Validation, Conceptualization, Methodology, Investiga
carbonatable materials. Carbonate binders are mainly composed tion, Data curation, Formal analysis, Review & Editing.
of CaCO3 and silica gel, which can be applied to produce concrete
materials and products.
Declaration of competing interest
(3) Magnesium oxide and magnesium silicate favor the sequestration
of CO2. The carbonate binders formed during the carbonation of
The authors declared that we have no conflicts of interest to this
magnesium materials include various forms of HMCs, the for
work. We declare that we do not have any commercial or associative
mation of HMCs is conducive to the evolution of interlocking
interest that represents a conflict of interest in connection with the work
network structure.
submitted.
(4) Apart from calcareous and magnesium materials, some calcium
or magnesium rich industrial by-products or waste materials can
Data availability
also be used to produce carbonate binders.
(5) The wet carbonation process is proposed recently and is widely
No data was used for the research described in the article.
applied to accelerate the carbonation of powder materials such as
recycled concrete fines and steel slag and develop a high valued
added carbonate binders. Acknowledgement
(6) By using industrial waste gas with different CO2 concentration,
application of carbonate binders to produce different construc This work was supported by the National Natural Science Foundation
tion products has been achieved in companies worldwide. of China under project No. 52078204 and 52278257.
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Cement and Concrete Research 175 (2024) 107352

Contents lists available at ScienceDirect

Cement and Concrete Research

Carbonate binders: Historic developments and perspectives

1. Introduction Given the substantial development and increased interest in low

Fig. 1. Schematic diagram of pre-conditioning and CO2 curing of concrete products.

Fig. 2. Schematic diagram of the wet carbonation of cement waste fines.

C3S Rapid ~20 %

β-C2S Slow ~30 %

γ-C2S Hardly ~50 %

Fig. 6. SEM images of CaCO3 samples induced by 11 selected amines [146].

4.1. Carbonation of magnesium-based materials

The magnesium sources with carbonation potential can be divided

FA 750–1000 5–40 0–10 Lime (CaO), portlandite (Ca(OH)2) 3.93–42.31 [245]

Fig. 14. CO2-SUICOM concept [62].

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