Journal of Building Engineering 79 (2023) 107779

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Journal of Building Engineering

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Accelerated carbonation of recycled concrete aggregates and its

implications for the production of recycling concrete
Andreas Leemann a, b, *, Frank Winnefeld a, Beat Münch a, Johannes Tiefenthaler c
a
Empa, Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland
b
School of Geography and Environmental Sciences, Ulster University, Coleraine, Northern Ireland, UK
c
Neustark AG, Berne, Switzerland

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

Keywords: During the demolition and recycling process the specific surface area per volume of concrete is
CO2 utilization significantly increased. As a result, the potential for CO2 absorption by carbonation of the cement
Carbonation hydrates is enhanced. In this study, recycled concrete aggregates (RCA) with varying moisture
Recycled concrete aggregates contents are carbonated with 100% CO2 at atmospheric pressure. The changes in the properties of
Recycling concrete RCA are characterized and they are used for the production of recycling concrete. There is only a
minor impact of carbonation on bulk density and water adsorption of the RCA. The accelerated
carbonation leads to the formation of calcium carbonate and decalcified calcium-silicate-hydrate
(C-S-H) present in patches on the surface of RCA particles. Using slurry instead of tap water
decreases concrete flow and generally increases compressive strength. Using carbonated instead
of uncarbonated RCA leads to a faster decrease of flow with time and to a higher compressive
strength of the recycling concrete compared to uncarbonated RCA. The higher strength linked to
the use of carbonated RCA offers the potential to decrease the clinker content of the recycling
concrete.

1. Introduction
Demolished concrete can be crushed to obtain recycled concrete aggregates (RCA) that are used to produce recycling concrete. The
motivation of this approach is to move towards a circular material flow in the construction industry and to preserve the limited sources
of natural aggregates [1–4]. Moreover, RCA have an additional potential to positively impact the environment. The cement hydrates
present in the RCA carbonate by absorbing atmospheric CO2 [5–10] Carbonation is a slow process that starts at the surface of concrete
components and the carbonation front advances with a square root of time law into the material [11–15]. It is assessed that about
11–30% of the geogenic CO2 emitted during cement clinker production is absorbed during the service life of concrete structures in
various European countries [6,8,16]. This is a substantial amount as cement production is responsible for about 6–8% of the
anthropogenic CO2 emissions [17–19]. During the demolition and recycling process the specific surface area of concrete is increased
substantially. The newly created surfaces make RCA susceptible for further carbonation. As the kinetics of carbonation and the degree
of carbonation are enhanced with increasing concentration of CO2 [20], the exposure of RCA to high CO2 concentration leads to a
substantial CO2 absorption [21–27]. Moreover, the bulk density of the RCA is increased and its water adsorption decreased, making it
more suitable for the production of recycling concrete [22,28–32].

* Corresponding author. Empa, Laboratory for Concrete & Asphalt, Dübendorf, Switzerland.
E-mail address: andreas.leemann@empa.ch (A. Leemann).

https://doi.org/10.1016/j.jobe.2023.107779
Received 4 July 2023; Received in revised form 11 September 2023; Accepted 13 September 2023
Available online 14 September 2023
2352-7102/© 2023 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/).
A. Leemann et al. Journal of Building Engineering 79 (2023) 107779

Starting in 2000, the use of RCA in concrete developed into an established approach in Switzerland [33–35] that was solidified in
the concrete industry by a national guideline first published in 2010 [36]. It classifies the different RCA components, regulates the
application of recycling concrete and defines correction factors for some key concrete properties. In the meantime, the potential of RCA
to absorb CO2 has been recognized by the concrete industry and a few companies have started activities in this direction.
The goal of this study is to investigate the potential of RCA to absorb CO2 and its implications for concrete production. The design of
the experiments takes into account the boundary conditions present in a concrete plant. RCA of different moisture levels are
carbonated and used to produce recycling concrete. Moreover, the effects of accelerated carbonation on the microstructure of RCA is
investigated. The study is conducted within the framework of DemoUpCARMA [37], a pilot project on CO2 management solutions for a
net-zero Switzerland. Simultaneously to the laboratory study, accelerated carbonation of RCA is implemented in a concrete plant
within the project.

2. Materials and methods

2.1. Materials
The slurry originates from a basin of the concrete plant where the waste water from cleaning the concrete and the concrete trucks is
retained. The slurry in the basin is stirred regularly to keep the particles in suspension and prevent layer formation at the bottom. The
density of the slurry was 1.064 g/cm3 as determined in a calibrated vessel with a volume of 1 L. The density of the slurry dried at 40 ◦ C
is 2.30 g/cm3. As such, 1 L of slurry has a solid content of 113 g. The solid and liquid content of the slurry was taken into account in the
mix design of the concrete.
In the concrete plant, the demolished concrete present in chunks of approximately 0.5–1.0 m in diameter is first stored outdoors in
unsheltered conditions exposed to the weather for a few months. Then it is crushed with a jaw crusher and sieved to produce RCA of the
grain size classes 0–16 mm and 16–32 mm. The RCA is first stored outdoors in unsheltered conditions for a few weeks depending on the
amount needed for concrete production. Then it is transported to the silos for concrete production. The RCA 0–16 mm is carbonated in
the silo with 100% CO2 obtained from a biogas plant, while the RCA 16/32 is not carbonated. The RCA for this study was taken from
the material transported to the silos before carbonation and delivered in big bags to the laboratory. After arrival in the laboratory, the
big bags were sealed to prevent carbonation.
The moisture content of the RCA 0–16 mm at the state of delivery was 6.0 mass-%, representing 120% of the water adsorption. The
measured grain size distribution of the 0–16 mm grain size class in the dry state is shown in Fig. 1. An additional sample was divided
into the grain size classes 0–4, 4–8 and 8–16 mm to determine bulk density and water adsorption. The results for these two parameters
are given in paragraph 3.2.
The sample size of RCA 0–16 mm used to determine CO2 absorption in a laboratory-scale reactor was 15.5 ± 1.0 kg. The samples
were first dried at 80 ◦ C for 24 h and packed into plastic bags afterwards. Then, an amount of water corresponding to values of water
adsorption of 30, 60, 100, 150 and 200% was sprinkled over the aggregates. The plastic bags were sealed air tight. The samples were
kept in the bags for 7 days to allow equilibration of the moisture content between the RCA particles. The moisture content at the state of
delivery was in the range of the tested moisture contents. The exposure time of RCA to CO2 in the silo at the plant is expected to be
between a few hours up to 24 h, depending on the amount of recycling concrete ordered by clients. Only during the weekend, longer
exposure times are achieved. Like in the plant, 100% CO2 was used in the laboratory to conduct the accelerated carbonation of RCA. In
addition to the grain size class 0–16 mm, one batch of the grain size classes 0–4, 4–8 and 8–16 mm was carbonated separately at a
moisture content corresponding to 100% of the water adsorption to determine CO2 absorption as a function of grain size.
The carbonation of RCA 0–16 mm used for concrete production was conducted at the moisture state of delivery in batches of 20 kg.
After carbonation the RCA were exposed to laboratory conditions for a week before used for concrete production. Their moisture

Fig. 1. Grain size distribution of RCA as delivered by the concrete plant corresponding to 46 mass-% of 0–4 mm, 41 mass-% of 4/8 mm and 13 mass-% of 8–16 mm.

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content corresponded to 50% of the water adsorption the time of production. This was taken into account in the concrete mix design.
Furthermore, 15 kg of RA 0–16 mm were spread in a container, mixed every week and exposed to natural carbonation for 7 months.
The temperature in the laboratory hall was between 19 and 25 ◦ C. Relative humidity and CO2 concentration in the air were not
recorded. Afterwards the sample was conditioned to a moisture state of 100% of the water adsorption and carbonated. Additionally, a
sample RCA 0–22 mm from another project [38] that was stored for 26 months spread in a container was conditioned and carbonated
as well.
Three samples were prepared for SEM. The grain size class 0.5–2.0 mm was obtained from RCA as delivered, from RCA after
carbonation with 100% CO2 (100% of water adsorption) and from the naturally carbonated RCA later exposed to 100% CO2. The
particles were dried, embedded in epoxy, ground, polished and carbon coated.

2.2. Mortar and concrete mix designs

For mortar production, the grain size class 0–2 mm was obtained by sieving RCA 0–16 mm after carbonation.
EN 196-1 standard quartz sand 0–2 mm [39] was used as natural aggregate in the mortar tests and alluvial sand and gravel for
concrete production. The latter consists mainly of limestone, sandstone and in smaller quantities siliceous limestone, dolomite, gneiss
and schist. The relative amounts of the different grain size classes used for concrete production were 40 mass-% of 0–4 mm, 15 mass-%
of 4–8 mm, 16 mass-% of 8–16 and 29 mass-% of 16/32 mm.
A Portland limestone cement (CEM II/A-LL 42.5 N) was used for mortar and concrete production. Its composition is shown in
Table 1. This cement typically contains 80 mass-% of cement clinker. As such 100 kg of CEM II/A-LL 42.5 N are linked to a geogenic
CO2 emission of 40.6 kg [40] and a total emission of 67.4 kg [41].
A commercial superplasticizer based on polycarboxylic ether was used for selected mortar and concrete mixtures.
The mix designs of the mortars and the concretes are given in Tables 2 and 3, respectively. The concrete mix design is based on the
Swiss standards [42] for type A concrete (minimum cement content of 280 kg/m3, maximum water-to-cement-ratio (w/c) of 0.65) and
type C concrete (minimum cement content of 300 kg/m3, maximum w/c of 0.50). The amount of RCA was kept constant at 60 mass-%
of the total aggregate agreeing with [36]. The recycling concrete was only produced with tap water, as no slurry is used for its pro­
duction in the concrete plant. 12 mortar prisms (40 × 40 × 160 mm3) and three concrete cubes 150 × 150 × 150 mm3 were produced
with each mixture to measure the compressive strength.

2.3. Methods
The RCA was placed in a barrel (volume of 75 L) without compaction and carbonated with a constant stream of 100% CO2 under
atmospheric pressure for the determination of CO2 absorption. A flexible tube connected the barrel with a 50 L steel bottle containing
liquid CO2. The CO2 stream entered the barrel at its bottom through two porous ceramic cylinders (diameter = 10 mm, length = 20
mm) as used for the ventilation of aquariums ensuring its homogeneous distribution. This allowed to ensure a homogenous CO2
distribution in the barrel. The barrel was placed on a scale with an accuracy of ± 0.001 kg. The flexible tube was disconnected from the
barrel for the periodic reading of the mass change. It was decided to carbonate RCA until an asymptotic behavior of CO2 absorption was
observed. This turned out to be after 70 min. The CO2 uptake was determined based on the mass change of the samples. The difference
in density between air and CO2 and the loss of moisture due to the CO2 stream was accounted for. The typical moisture loss was
determined on a RCA sample with a moisture content of 100% WA using N2 instead of CO2 resulting in a water loss of 0.028 kg in 70
min. This water loss corresponds to about 3.5% of the water present in the sample at a moisture content corresponding to 100% of
water adsorption. As such, it can regarded as negligible. As the portlandite content of the RCA before and after carbonation were not
determined, the potential water loss due to portlandite carbonation like it was performed in Ref. [43] cannot be taken into account. In
order to determine the repeatability of the CO2 absorption, three samples with a moisture content of 100% WA were carbonated,
leading to values of 11.22 ± 0.17 kg/t of dry RA.
Bulk density and water adsorption were measured first in the uncarbonated state according to EN 1097-6 [44]. The authors are
aware that the EN 1097-6 uses the term “water absorption”. However, the major part of the water is adsorbed by the external and
internal surfaces of the RCA. In contrast to that, CO2 is chemically bound in the cement hydrates of the RCA. Therefore, the authors
prefer to use the term “water adsorption” to clearly distinguish the process to true absorption like in carbonation.
After the test, the samples were conditioned to 100% of the water adsorption, carbonated and reused for the determination of bulk
density and water adsorption, avoiding possible effects of sample variation.
The density of the slurry was determined using a calibrated vessel with a volume of 1 L.
The microstructure of carbonated RCA particles was investigated using a FEI Quanta 650 in the high vacuum mode (pressure of
3.5–5.0 × 10− 6 Torr). An acceleration voltage of 12.5 kV, a spot size of 4.5 and a beam current of 155–170 μA were employed to
acquire back-scattering-electron (BSE) images. EDS was conducted with a Thermo Noran Ultra Dry 60 mm2 detector and Pathfinder X-
Ray Microanalysis Software. For the single point analysis, the same setting as for image acquisition were employed. Acceleration

Table 1
Composition of the CEM II/A-LL. LOI = loss on ignition, CO2 was calculated from total carbon analysis.

type CaO SiO2 Al2O3 Fe2O3 Cr2O3 MnO TiO2 P2O5 MgO K2O Na2O SO3 LOI CO2

[mass-%]

CEM II/A-LL 60.6 17.1 4.27 2.68 0.005 0.05 0.24 0.14 1.80 0.84 0.13 3.12 8.90 8.25

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Table 2
Mortar mix design. The mortar mixtures are named as follows, R1- UC2: 1 = recycling (R) or primary (P) mortar, 2 = carbonated (C)) or uncarbonated (UC) RA. SP =
superplasticizer.

components mortar P mortar R–UC mortar R–C

[g] [g] [g]

CEM II/A-LL 900 900 900

water 450 529 529
SP – 3.5 2.5
NA 0–2 mm 2700 1350 1350
RCA-UC 0–0.5 mm – 540 –
RCA-UC 0.5–1.0 mm – 338 –
RCA-UC 1–2 mm – 473 –
RCA-C 0–0.5 mm – – 540
RCA-C 0.5–1.0 mm – – 338
RCA-C 1–2 mm – – 473

Table 3
Concrete mix design. The water content for w/c is equal to total water minus the water adsorption of NA and RCA. The concrete mixture are named as follows, R1-A2-
UC3-T4: 1 = recycling (R) or primary (P) concrete, 2 = type A or C concrete, 3 = carbonated (C) or uncarbonated (UC) RA, T = tap (T) water or slurry (S).

Concrete RCA 0–16 UC RCA 0–16 C RCA 16/32 UC NA CEM II/A-LL Water type SP w/c

[kg/m3] [kg/m3] [kg/m3] [kg/m3] [kg/m3] [− ] [kg/m3] [− ]

P-A-T – – – 1910 280 tap – 0.61

P-A-S – – – 1883 280 slurry – 0.61
R-A-UC-T 716 – 337 697 290 tap – 0.56
R-A-UC-S 706 – 332 687 290 slurry – 0.56
R-A-C-T – 719 337 697 290 tap – 0.56
P-C-T – – – 1938 310 tap 0.6 0.48
P-C-S – – – 1915 310 slurry 0.6 0.48
R-C-UC-T 725 341 706 320 tap 2.2 0.44
R-C-UC-S 718 – 338 698 320 slurry 2.2 0.44
R-C-C-T – 729 341 706 320 tap 2.2 0.44

voltage and spot size were increased for element mappings to 20 kV and 5.0, respectively. Phase clustering was performed according to
Ref. [45].
The mortars were produced in a Hobart mixer and their compressive strength were measured after 2, 7, 28 and 91 days according to
Ref. [39]. The concrete was produced in an Eirich 75 L mixer. The components were first dry mixed for 60 s, before the water and the
superplasticizer were added. After their addition, the concrete was mixed for 90 s. Concrete flow [46] was determined 5, 20 and 50 min
after production. Bulk density [47] and air void content [48] were measured 5 min after production. Compressive strength was
determined after 2, 7 and 28 days [49]. The standard deviation of compressive strength as determined on three cubes of 40 different
concrete mixtures is ± 0.8 MPa. This value is stated in the respective figures as “representative error".

Fig. 2. CO2 absorption of RA 0–16 mm with different moisture contents expressed as percentage of the water adsorption in kg per ton of dry RCA as a function of
exposure time.

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3. Results
3.1. CO2 absorption
While the CO2 absorption by the RCA does not show large differences at a moisture content corresponding to 60–200% of the water
adsorption (Fig. 2), the value nearly doubles at a lower moisture content (30% of the water adsorption). It rises from ⁓ 11 to ⁓ 21 kg
CO2/t of RA within 70 min of exposure.
The RCA used for concrete production were carbonated at the moisture state of delivery (120% of WA) resulting in an average of
11.3 kg CO2/t of dry RCA. As such, the amount of carbonated RCA used for the production of concrete R-A-C-T and R-C-C-T (Table 3)
incorporates 8.0 kg CO2/m3 of recycling concrete in average.
CO2 absorption of RCA significantly depends on its grain size (Fig. 3). The sand absorbs considerably more, with a value of 21.6 kg/t
of dry RCA compared to the coarser grain size classes with values of 1.5 (4–8 mm) and 0.6 (8–16 mm) kg/t of dry RCA.
The two sample pre-carbonated for 7 (RCA 0–16 mm) and 26 months (RCA 0–22 mm) absorb considerably less CO2 during the
accelerated carbonation (Fig. 4). The value of RA 0–16 mm decreases 64% from 11.28 to 4.05 kg t of dry RA. RA 0–22 mm absorbs even
less CO2, with 2.12 kg/t of dry RCA. However, here no reference value for the condition before natural carbonation like in the case of
RA 0–16 mm is available.

3.2. Bulk density and water absorption

Bulk density slightly increases and water adsorption decreases with increasing grain size. Carbonation leads only to a minor in­
crease of bulk density and a minor decrease of water adsorption in the sand (Table 4). There is no measureable effect of carbonation on
the larger grain size classes.

3.3. Microstructure
The microstructural investigation reveals that the sand particles of the studied size (0.5–2 mm) exposed to accelerated carbonation
exhibit patches in the cement paste with a decreased backscattering contrast at their surface (Fig. 5). The cement paste of some small
particles is completely altered (Fig. 6A). These patches are completely absent in the non-carbonated sample. Although they are less
frequent in the sample that was pre-carbonated naturally before accelerated carbonation, they still occur. EDS point analysis reveals
that the phases with the decreased backscattering contrast consist mainly of decalcified calcium-silicate-hydrate (C-S-H) with
aluminum as a minor component and small amounts of silica gel containing aluminum, magnesium and potassium. On the other hand,
the altered patches contain layers and clusters with a very high backscattering contrast (Fig. 6A) consisting of CaCO3. Phase clustering
based on element maps makes these two major products of accelerated carbonation visible (Fig. 6B).
The difference in carbonation between the bulk cement paste in the particles and the described patches can be shown best by the
analysis of the C-S-H present as inner product (formed within the boundaries of the former clinker grains). Here, C-S-H composition is
typically homogeneous and there is less interference with other cement hydrates such as portlandite, ettringite and monocarbonate,
which are typically intermixed with C-S-H like at other locations in the cement paste. C-S-H in the inner product shows a marked
difference in the patchy zones of decreased backscattering density and in the zones with higher backscattering density not altered by
accelerated carbonation. The Si/Ca-ratio in the patchy zones ranges from 1.1 to 2.5 and in the other areas of the particles between 0.53
and 0.75 (Fig. 7). The points with a Al/Ca-ratio > 0.2 may indicate the occurrence of intermixed Al(OH)3 resulting from the
carbonation of ettringite and monocarbonate. Additionally, there are amorphous phases intermixed with silica gel with a relatively
high potassium and aluminum content pointing towards precursors of zeolites.

Fig. 3. CO2 absorption during an exposure of 70 min in kg per ton of dry RCA of the different grain size classes.

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Fig. 4. CO2 absorption in kg per ton of dry RCA of samples pre-carbonated at atmospheric CO2 level for 7 (RCA 0–16 mm) and 26 months (RCA 0–22 mm).

Table 4
Bulk density in the dry state and water adsorption of the RCA in the uncarbonated (UC) and carbonated (C) stage. Note: RCA 16–32 mm was only used in the
uncarbonated state for concrete production.

0–4 mm 4–8 mm 8–16 mm 16–32 mm

UC C UC C UC C UC
3
Bulk density [g/cm ] 2.332 2.357 2.400 2.389 2.419 2.414 2.408
Water adsorption [mass-%] 5.86 5.13 4.50 4.53 3.97 3.92 3.86

Fig. 5. BSE-image of RCA sand particles after accelerated carbonation with patches at their surface showing a decreased backscattering contrast (indicated by
white arrows).

3.4. Mortar
The substitution of quartz sand with uncarbonated and carbonated RCA of the same grain size leads to a decrease of compressive
strength (Fig. 8). However, the decrease is less pronounced in the case of mortar R–C. At the age of 28 days, typically used as reference
for compressive strength, the value of mortar R–C is only 7.4% lower than the one of mortar P. The compressive strength of mortar
R–UC is 19.8% lower.

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Fig. 6. RCA sand particle after carbonation with 100% CO2 (A) as BSE-image and as phase map based on element maps showing decalcified C-S-H and calcite as main
alteration products (B). Quartz (SiO2) and feldspar are components of the primary aggregate particles enclosed in the RCA particle. SiO2 additionally occurs as silica
gel resulting from complete C-S-H carbonation. Ferrite is an unhydrated phase of the cement clinker.

Fig. 7. Al/Ca-ratio as a function of Si/Ca-ratio of C-S-H not altered by accelerated carbonation and C-S-H decalcified by accelerated carbonation present in the patches
at the edge of particles as pointed out in Fig. 5. The red dot indicates the typical composition of C-S-H formed during Portland cement hydration.

Fig. 8. Mortar P with 100% NA and mortar R containing 50 mass-% RA in either uncarbonated (UC) or carbonated (C) form.

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3.5. Concrete
An overview of the fresh and hardened concrete properties is given in Table 5.
The combination of NA and slurry leads to a lower concrete flow in concrete P-A-S and in particular P-C-S compared to concrete P-
A-T and P-C-T produced with tap water (Fig. 9A). The relative decrease of concrete flow with time is similar for both concrete types.
However, compressive strength at all measured ages is increased by the use of the slurry, in more pronounced way for lower quality
type A concrete (Fig. 9B).
Combining uncarbonated RCA and slurry in concrete R-A-UC-S has the same effect as for the concrete P (Fig. 10A). Concrete flow is
decreased significantly compared to the concrete R-A-UC-T produced with tap water. Concrete R-A-UC-S displays such a poor
workability after 20 min that concrete flow was hardly measureable. When carbonated RCA is used in combination with tap water in
concrete R-A-C-T, the flow decreases faster than in concrete R-A-UC-T. In general, the decrease of workability of concrete R occurs
slightly faster compared to concrete P.
The use of carbonated RCA and slurry instead of tap water leads to an increase in compressive strength compared to concrete R-A-
UC-T (Fig. 10B).
The effect of the slurry and of carbonated RCA in concrete R–C is the same as in type A concrete. The slurry leads to a considerably
lower flow and the carbonated RCA causes a faster decrease of flow (Fig. 11A). While the increase of compressive strength is only minor
in the case of the slurry, the carbonated RCA in concrete R-C-C-T leads to a more significantly increased value at 28 days compared to
concrete R-C-UC-T (Fig. 11B).

4. Discussion
4.1. Carbonation
4.1.1. CO2 absorption
CO2 absorption of RCA shows a relatively small influence of the moisture content from 60 to 200% of the water absorption. Instead,
at 30% of the water adsorption, RCA absorbs significantly more CO2: 21 kg/t of CO2 per dry mass of RCA compared to 10–12 kg/t at
higher moisture content. This clearly shows that carbonation proceeds faster in relatively dry concrete [11–15]. However, the RCA had
a moisture content of 120% of the water adsorption at the state of delivery. The exposure of the demolished concrete and RCA to the
weather in unsheltered conditions (paragraph 2.1) is typical for Switzerland, resulting in moisture contents of the RCA in the range of
100–200% of the water adsorption [38]. As a result, it can be expected that a CO2 absorption of 10–12 kg/t of dry RCA can be achieved
by accelerated carbonation of the grain size class 0–16 mm in an industrial set-up. Moist RCA dry very slowly, when stored in sheltered
conditions [38]. Accelerated drying of RCA to a lower moisture content would increase their CO2 absorption potential. However, this
would be linked to energy consumption and CO2 release. This situation is specific to Switzerland and may be different in countries with
a drier climate.
After crushing, RCA are exposed to natural carbonation, which decreases their CO2 absorption potential by accelerated carbonation
as shown by the results obtained using naturally pre-carbonated samples. However, the two pre-carbonated samples may be regarded
as a worst case scenario as they were exposed to natural carbonation as thin layers for several months. They still reach a CO2 absorption
of 2–4 kg/t of dry RCA, because the degree of carbonation of cement hydrates increases with increasing CO2 level [20]. RCA exposed to
natural carbonation in a pile for 6–8 months absorbs between 5.4 and 12.7 kg of CO2 per ton of RCA [38]. It can be regarded as a benefit
for total CO2 absorption that accelerated carbonation is still able to increase these values. However, the benefit for the producer of
artificially carbonated RCA is lower, as the declarable CO2 absorption decreases.
The amount of absorbed CO2 during accelerated carbonation in relation the geogenic CO2 emission resulting from clinker pro­
duction can be assessed. About 95% of the concrete produced in Switzerland falls into the types A, B and C. The minimum cement
content and maximum w/c for these types is defined in the Swiss standards [50]. Based on these prescription, an average cement
content of 300 kg/m3 and w/c of 0.55 can be assumed for the RCA derived from such concrete. Because demolished buildings are

Table 5
Overview of the concrete properties. R1-A2-UC3-T4: 1 = recycling (R)) or primary (P) concrete, 2 = type A or C concrete, 3 = carbonated (C)) or uncarbonated (UC) RA, T
= tap (T) water or slurry (S).

Concrete Flow Bulk density Air voids fc

[cm] [kg/m3] [vol-%] [MPa] [MPa] [MPa]

5 min 20 min 50 min 2d 7d 28d

P-A-T 45.5 40.5 38 2366 2.5 13.8 20.3 25.2

P-A-S 39 35 31 2375 2.5 15.8 24.3 28.5
R-A-UC-T 47 44 38 2280 2.1 14.5 23.4 28.8
R-A-UC-S 34.5 31 -a 2266 2.2 16.4 24.9 30.3
R-A-C-T 48.5 39 33 2282 2.6 16.0 25.2 31.6
P-C-T 50.5 44.5 38 2405 2.7 25.5 37.3 42.4
P-C-S 31.5 29 -a 2421 2.3 27.4 39.4 43.1
R-C-UC-T 47.5 44.5 34.5 2345 1.5 24.9 36.8 42.1
R-C-UC-S 33.5 28 -a 2322 1.8 24.9 37.1 43.5
R-C-C-T 46 36.5 30.5 2325 1.7 25.3 37.4 47.3
a
Flow too low to be measurable.

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Fig. 9. Concrete flow (A) and compressive strength (B) as a function of time of concrete P produced with either tap water or slurry.

typically several decades old, it can be further assumed that the cement used was a plain Portland cement without supplementary
cementitious materials, the dominant cement type until about 30 years ago in Switzerland. The geogenic CO2 emission per ton of
concrete is directly related to the CaO content of the cement in the concrete and can be calculated using the following numbers and
equation:
300 = cement content in kg/m3
0.95 = relative clinker content in Portland cement
0.64 = relative CaO content in clinker
0.79 = ratio between molar mass of CO2 and CaO
2.4 = concrete density

CO2,geogenic = (300 × 0.95 × 0.64 × 0.79)/2.4 = 60 kg (1)

Consequently, a CO2 absorption of 10–12 kg/t of dry RCA during accelerated carbonation represents a relative value of 17–20% of
the geogenic CO2 emission caused by production of the cement used to produce the source concrete of the RCA. However, it has to be
pointed out that the grain size class 16–32 mm is not exposed to accelerated carbonation due to its low potential for CO2 absorption. As
this grain size class accounts for about 30% of the RCA produced in the specific plant, the percentage of absorbed CO2 in relation to the
geogenic emission decreases to 12–14%.

4.1.2. Microstructure
When a mortar or concrete produced with Po is carbonated, the total porosity is decreased and the mean pore diameter is increased
[15,51]. However, bulk density and water absorption in the grain size classes 4–8 and 8–16 mm do not change at all and there is only a
minor change in the sand at the chosen duration of carbonation. This clearly shows that there is no densification of the particles by
carbonation, indicating CO2 absorption limited to cement paste close to the surface. This is confirmed by the analysis of the micro­
structure, where the formation of porous patches is restricted to the surface of particles and reaches a depth of up to 1 mm. The
observed de-calcification of C-S-H and disappearance of portlandite, accompanied by the formation of calcite rims and clusters, clearly

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A. Leemann et al. Journal of Building Engineering 79 (2023) 107779

Fig. 10. Concrete flow (A) and compressive strength (B) as a function of time of concrete R-A.

shows that calcium dissolution followed by CaCO3 precipitation occurs. The microstructure resembles the one formed by an attack of
carbonic acid on concrete [52,53]. CO2 dissolves in water contained in the RCA and forms carbonic acid, leading to portlandite
dissolution and C-S-H decalcification [54]. When the CO2 concentration is decreased after carbonation, the reverse reaction takes place
and the dissolved calcium is precipitated as CaCO3. The patchy occurrence of the decalcified C-S-H may be the result of
particle-to-particle contacts that restrict the access of CO2. The presence of strongly decalcified C-S-H and possibly Al(OH)3 has im­
plications for the reuse in RC. These phases react with portlandite formed by the hydration of the cement in the newly produced
concrete [55–57]. Small particles <125 μm may act like a supplementary cementitious material and improve compressive strength
[56,58–61]. A reaction on the surface of larger particles can improve the binding between cement paste and RCA [62]. In the case of
the RCA pre-carbonated under natural conditions before accelerated carbonation, the CO2 absorption is relatively low, but the
modification of the microstructure will still have a beneficial effect on concrete strength.
There is a discrepancy between the lack of densification of the RCA as described above and the densification and reduced water
adsorption reported in other studies [22,25,28–30,32,63]. This situation is caused by the way RCA carbonation is conducted. In the
referenced studies RCA were preconditioned at relative humidity between 50 and 70%. Carbonation took place at similar relative
humidity levels with 100% CO2 and elevated gas pressure in some cases. As a result, the degree of carbonation of the RCA achieved is
very high, which explains the reported changes in their characteristics. Various laborious and sophisticated procedures for such
accelerated carbonation of RCA are summarized in Ref. [25]. It has to be pointed out that many of these procedures seem to be difficult
or impossible to implement in a concrete plant. Additionally, every process step is linked to a certain energy consumption and CO2
emission. It is an advantage of the simple approach chosen for this project that it is able to reach a carbon removal efficiency of 93.6%
as shown by life cycle assessment [64]. As such, the different process steps needed for the carbonation process amount to 6.5% in
relation to the CO2 absorbed by the RCA.

4.2. Mortar and concrete properties

Compressive strength and static E-modulus of quartzite used as natural aggregates in the mortar can reach values of > 300 MPa and
60 GPa, respectively [65]. A concrete with a compressive strength of 35 MPa typically displays a static E-modulus in the range of 30
GPa [66]. The differences in the mechanical properties of natural quartz sand and RA explains the decrease of the compressive strength
between mortar P and mortar R. However, mortar R–C reaches a higher strength than mortar RA-UC increasing from +3.1% at the age

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A. Leemann et al. Journal of Building Engineering 79 (2023) 107779

Fig. 11. Concrete flow (A) and compressive strength (B) as a function of time of concrete R–C.

of 1 day to +16.4% at the age of 91 days. As the accelerated carbonation has only a minor effect on the bulk density of the RCA, this
difference has to be attributed the formation of de-calcified C-S-H during carbonation and its ensuing reaction with Ca(OH)2 in mortar
R–C as indicated in Refs. [55,56] and confirmed in Ref. [57].
The lower flow of both concrete P and R produced with slurry instead of tap water is likely caused by the increase of the specific
surface area of the solids due to the very fine particles suspended in the slurry. On the other hand, they accelerate cement hydration
and therefore can increase the compressive strength [56]. When the lower flow is counteracted by the use of a higher w/c, the benefit
of the strength increase is lost. If the lower flow is counteracted by the use of a superplasticizer or an increase in its dosage, compressive
strength can be expected to be not affected. It has to be pointed out that the use of the slurry increases mainly the strength of concrete P.
Possibly, there are already many fine grained particles similar to the ones in the slurry attached to the coarser RCA particles causing the
same effect on cement hydration. As a result, the slurry has only a slight impact on strength development of concrete R.
Although the use of carbonated RCA in concrete R has no impact on initial flow (value 5 min after production), the values are
decreasing faster with time compared to the ones of concrete with uncarbonated RCA. This is likely linked to the participation of the
decalcified C-S-H in cement hydration and was already observed in Ref. [57]. On the other hand, this goes together with a strength
increase of the concrete with carbonated RCA. If the effect on concrete flow can be overcome with superplasticizers or retarders
without affecting the strength, there is the potential to adapt the concrete mix design to the strength-increasing effect of carbonated
RCA [67]. In paragraph 4.1.1 the CO2 absorption of the RCA is brought into context to the CO2 emission linked to the source concrete of
the RCA. However, the potential for a CO2 reduction due to the CO2 absorbed by the RCA and the adaption of the concrete mix design
due to the reactivity of the carbonated RCA can be assessed as well in regard to the production of the recycling concrete. If the volume
of cement paste (cement and water) is kept constant and the relation between w/c and compressive strength established in Ref. [35] is
considered, the cement content can be reduced between 4 (type A concrete) and 8 (type C concrete) mass-%, respectively. Compared to
a recycling concrete produced with uncarbonated RCA resulting in identical strength, the use of carbonated RCA can lead to an overall
reduction of the geogenic CO2 emission [40] of 10–14%, if the CO2 captured by the accelerated carbonation of the RCA (chapter 3.1.1)
and the reduction of the cement content are considered.

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A. Leemann et al. Journal of Building Engineering 79 (2023) 107779

5. Conclusions
Accelerated carbonation with 100% CO2 was performed on RCA. The effect of carbonation on the properties and microstructure of
the RCA was investigated. Furthermore, the impact of slurry, uncarbonated and carbonated RCA on the properties of mortar and
concrete were studied. The results allow to draw the following conclusions for the carbonated materials:
• The CO2 absorption of RCA 0–16 mm exposed to accelerated carbonation with 100% CO2 for 70 min in the laboratory ranges from
10.2 to 12.7 kg/t of dry RCA at a moisture content corresponding to 60–200% of the water adsorption. Such moisture contents
reflect the ones to be expected of RCA produced in concrete plants. At a moisture content equaling 30% of the water adsorption CO2
absorption increases considerably to a value of 21.2 kg/t of dry RCA.
• The sand 0–4 mm absorbs 14 times more CO2 than the grain size class 4/8 mm and 35 times more than the grain size class 8/16 mm.
• A pre-carbonation of RCA at natural CO2 level for 7 months in sheltered conditions decreases absorption to 4.0 kg/t of dry RCA
(moisture content of 100 % of the water adsorption).
• The impact of accelerated carbonation on the bulk density and water adsorption of RCA is minor.
• Accelerated carbonation leads to a patchy decalcification of C-S-H and the formation of CaCO3 layers and clusters on the surface of
RCA particles.
• The decalcified C-S-H is potentially reactive and can participate in cement hydration in a newly produced recycling concrete.
As the composition of RCA can vary, the determined values for CO2 absorption can be expected to vary as well between different
RCA.
The use of slurry and RCA have the following impact on mortar and concrete properties:

• The high surface area of the particles suspended in the slurry cause a significantly lower concrete flow both in primary concrete P
produced with natural aggregates and in recycling concrete R produced with RCA when compared to identical mixtures produced
with tap water.
• In concrete P the slurry increases compressive strength compared to the reference concrete produced with tap water. This effect is
less pronounced in concrete R.
• Carbonated RCA lead to a faster decrease of concrete flow and an increase the compressive strength of mortar and concrete. This is
attributable to the participation of decalcified C-S-H in cement hydration.
• The participation of decalcified C-S-H formed by accelerated carbonation in cement hydration has the potential to reduce the
cement clinker content in the mix design of recycling concrete. A prerequisite for such an adaption is the use of optimized retarders
or superplasticizers that offset the faster decrease in concrete flow.

Author statement
Andreas Leemann: Conceptualization; Formal analysis; Funding acquisition; Investigation; Methodology; Project administration;
Resources; Validation; Visualization; Roles/Writing - original draft; Writing - review & editing. Frank Winnefeld: Conceptualization;
Formal analysis; Funding acquisition; Investigation; Methodology; Resources; Validation; Roles/Writing - original draft; Writing -
review & editing. Beat Münch: Investigation; Methodology; Software; Validation; Visualization; Writing - review & editing. Johannes
Tiefenthaler: Conceptualization; Funding acquisition; Methodology; Project administration; Writing - review & editing.

Declaration of competing interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing in­
terests: Andreas Leemann reports financial support was provided by Swiss Federal Office of Energy.

Data availability

Data will be made available on request.

Acknowledgements
The authors would like to acknowledge Pietro Lura (Empa) for reviewing the manuscript. The Swiss Federal Office of Energy and
the Swiss Federal Office for the Environment are acknowledged for partly funding this study within the framework of the
“DemoUpCarma” project, and Kästli Bau AG, Rubigen (Switzerland) for providing the recycled concrete aggregates and the concrete
slurry waste. Additionally, the authors would like to thank the two anonymous peer reviewers for their work.

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