Cement and Concrete Composites 104 (2019) 103360

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Cement and Concrete Composites

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Carbonation treatment of recycled concrete aggregate: Effect on transport T

properties and steel corrosion of recycled aggregate concrete
Bao Jian Zhana, Dong Xing Xuana, Weilai Zenga,b, Chi Sun Poona,*
a
Department of Civil and Environmental Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong
b
Institute of Structural Engineering, Zhejiang University, Hangzhou, Zhejiang, China

A R T I C LE I N FO A B S T R A C T

Keywords: Old cement mortars attached on recycled concrete aggregates (RCA) seriously affects the durability of the re-
Cement mortar cycled aggregate concrete (RAC). Revealing the variation of the transport properties of cement mortar after
Carbonation subjecting to accelerated carbonation treatment is crucial with respect to understanding the effects of carbonated
Transport properties RCA on the durability of RAC. In this paper, cement mortars were used to study the transport properties after
Corrosion
they were treated by accelerated carbonation. The corrosion behavior of steel bars in the concrete incorporating
Recycled aggregate
the carbonated RCA was also evaluated. The experimental results indicated that the water absorption and
sorptivity, resistance to chloride ion penetration, as well as the bulk electrical conductivity of the cement mortar
was decreased after subjecting the accelerated carbonation treatment. Extending the treatment from 1 day to 7
days only resulted in a marginal improvement of the transport properties. A significant decrease in the local
porosity at the edge of cement mortar determined by Scanning electron microscopy-backscattered image was
observed, agreeing well with the concentrated calcium carbonate (CC) contents detected in the surface layer by
TGA. The determination of the spatial gradients of the porosity and carbonates/portlandite contents illustrated
that even only with the external layer (0–10 mm) carbonated, a considerable improvement of transport prop-
erties of the cement mortar could still be achieved. The corrosion test in the new concrete prepared with the
carbonated RCA also confirmed that the corrosion resistance of steel bars in the RAC was improved.

1. Introductions
Recycled concrete aggregates (RCA) derived from demolition con-
crete can be regarded as an alternative coarse aggregate. They are ty-
pically blended with natural coarse aggregate for use in new con-
struction materials, e.g. in concrete. The use of 100% RCA to replace
natural coarse aggregates in new concrete, unless carefully managed
and controlled, is likely to have a negative influence on most concrete
properties due to the presence of adhered old cement mortar on the
surface of RCA, which could contain a significant amount of fully hy-
drated cement paste. Compared to the typical natural aggregate (NA)
used in concrete, the adhered cement mortar on the RCA has a lower
density, higher water absorption and lower abrasion resistance [1–3].
Besides, the RCA also contains more microcracks caused by the
crushing process, and more interfacial transition zones (ITZs) which are
the original ITZs between the old cement mortar and the virgin ag-
gregate in RCA [4,5]. These differences in RCA and NA characteristics
have been widely reported as the main cause leading to the inferior
mechanical and durability properties of the new concrete [6,7].
For the recycled aggregate concrete (RAC) with a given mix for-
mula, its durability is severely affected by the content and properties of
RCA, and the deterioration of durability properties is more pronounced
than the mechanical properties with increasing contents of RCA [8].
Previous studies have reported that a significant increase in water
permeability, sorptivity and water absorption capacity were observed
for the concrete when over 50% of NA was replaced by RCA [9,10]. The
RCA with a higher content of adhered cement mortars can also lead to
higher capillary water absorption of the resulted RAC [11]. Further-
more, the increase of RCA content generally deceases the resistance to
chloride ions penetration of the concrete. Duan and Poon also found
that reducing the amount of adhered cement mortars would increase
the chloride ion penetration resistance of RAC [12]; while the RCA
originated from a higher strength of concrete could render the resulted
RAC a higher resistance to Cl− ions penetration [13]. Previous works
have shown that there are more capillary channels in the RAC than in
the NAC, due to the introduction of ITZs between the natural aggregates
and old cement mortars, and microcracks in the RCA [7,14,15], as
shown in Fig. 1(a). The porous nature and the presence of microcracks

*
Corresponding author.
E-mail address: cecspoon@polyu.edu.hk (C.S. Poon).

https://doi.org/10.1016/j.cemconcomp.2019.103360
Received 3 May 2019; Received in revised form 27 June 2019; Accepted 2 July 2019
Available online 04 July 2019
0958-9465/ © 2019 Elsevier Ltd. All rights reserved.
B.J. Zhan, et al. Cement and Concrete Composites 104 (2019) 103360

Table 1
Chemical composition of OPC.
Oxides CaO SiO2 Al2O3 Fe2O3 MgO Na2O K2O SO3 LOI

wt. % 63.15 19.61 7.52 3.32 2.14 0.13 0.32 2.03 2.14a

a
The loss on ignition of OPC was measured according to BS EN 196–2.

carbonated RCA.

2. Experimental program

Fig. 1. Schematics of microstructure of: (a) as received RCA, and (b) RCA after 2.1. Transport properties of carbonated mortar
carbonation treatment.

2.1.1. Materials and samples preparation

play a crucial role on governing the mass transport properties of the An ordinary Portland cement (Green Island Cement (Holdings) Ltd.)
RCAs. Meanwhile, the average content of attached cement mortars in complying with ASTM Type I was employed for preparing the cement
the RCAs normally vary in a range from 20% to 70% (by weight), de- mortar in this study. The chemical composition of the OPC was de-
pending on the particle size, crushing process and strength grade of termined by X-ray fluorescence (XRF, Rigaku Supermini 200), and the
their parent concrete [16]. Thus, it cannot be ignored that the transport results are shown in Table 1. The density of OPC is 3.16 g/cm3 and its
properties of the old cement mortar attached to the RCAs exert a con- specific surface area is 3490 cm2/g.
siderable influence on the durability behaviors of the new RAC. Natural river sand (< 4.75 mm) with a specific gravity of 2.60 and a
During the last decade, there have been numerous attempts to try to fineness modulus of 2.89 was used as aggregates. Cement mortar was
strengthen the attached cement mortar and thus enhance the properties prepared with a mix formulation of cement: sand: water = 1: 2: 0.6,
of RCA, and they have been thoroughly summarized in some previous according to the fabrication procedures described in BS EN 196–1:2016.
studies [3,17,18]. A CO2 curing method has been proposed recently by Cylindrical samples were cast in steel molds with two different sizes:
Kou et al. [19] and Zhan et al. [20], aiming to densifying the old cement Ø 50 × 100 mm and Ø 100 × 200 mm. All the mortar samples were
mortar attached to the RCA through the accelerated carbonation reac- demolded after 24 h and then soaked in a tap water tank for 3 months at
tion. These investigations found that the accelerated carbonation re- 23 ± 1 °C.
actions enhanced the physical and mechanical properties of recycled After the curing period, the cylindrical specimen (Ø 50 × 75 mm)
mortar/concrete aggregates with particle size ranging from 5 to 20 mm were sectioned from the Ø 50 mm cylinders by cutting away the uneven
by reducing the total porosity and water absorption capacity, and in- trowelled end (see Fig. 2 (a)), for the subsequent accelerated carbona-
creasing the apparent density. This is mainly attributed to the carbo- tion treatment, and testing of water absorption, sorptivity and apparent
nation of portlandite (CH), forming calcium carbonates with an in- chloride diffusion coefficient. Similarly, 50 mm thick discs were sec-
creased solid volume which fills the pore spaces and thus densifies the tioned from the center of the Ø 100 mm cylinders (see Fig. 2 (b)) for
microstructure [21], as illustrated in Fig. 1(b) (assuming the old cement testing the resistance of chloride penetration ability and electrical
mortar is fully carbonated). Furthermore, by using the accelerated conductivity before and after the carbonation treatment.
carbonation treatment, the mechanical properties of the resulted new
concrete were generally improved [3,18,19,22]; the microhardness of
2.1.2. Accelerated carbonation treatment
the new ITZ around the carbonated RCA was found to be higher [3]; the
Accelerated carbonation treatment of the cement mortar was car-
durability of the new concrete was improved by reducing the chloride
ried out by using two steps: preconditioning and CO2 curing. Prior to
ion permeability and gas permeability [23,24].
CO2 curing, the sectioned specimen described above were precondi-
Nearly all of the previous studies mentioned above focused either on
tioned in an environmental chamber at 25 ± 1 °C and 50 ± 1% RH for
the physical and mechanical properties of the carbonated RCAs them-
one week, in order to lower the water saturation degree of the samples
selves, or on the mechanical performance and durability of the concrete
to facilitate the carbonation reactions [34,35]. Then, the specimen were
prepared with the carbonated RCA; but no studies have assessed the
transferred into a CO2 curing chamber [36,37], and subjected to the
impact of accelerated carbonation treatment on the transport properties
accelerated carbonation under 100% CO2 atmosphere at a pressure of
of RCAs themselves.
1 bar for 1 day and 7 days. The conditioning regimes for different
The transport properties of RCA/concrete are mainly controlled by
samples are presented in Table 2. For the reference samples, the total
the characteristics of its pore network, including total porosity, pore
size distribution, pore connectivity and tortuosity, as well as the sa-
turation degree by water. It has been demonstrated that calcium car-
bonate formed during the carbonation process is barely soluble in water
and thus contributes significantly to clogging of the pore network,
eventually leading to marked changes of the transport properties of
liquids and gases through the carbonated cement paste [25,26]. De-
waele et al. [27] found the permeability of a cement grout decreased by
several orders of magnitude after carbonation under the pressurized
CO2-rich water. A significant decline in permeability of the carbonated
concrete has also been reported by Claisse et al. [28]. Similar results
have also been reported elsewhere [29,30]. On the contrary, there are
also some previous studies revealing an increase in chloride diffusion
coefficient and oxygen permeability for the carbonated cement blends
(PFA, GGBS) [31–33]. This current work attempts to assess the effects
of accelerated carbonation treatment on the transport properties of RCA Fig. 2. Sketch of test specimen sectioned from the cylindrical samples: (a) Ø
and the risk of steel corrosion in the new concrete prepared with the 50 mm specimen; (b) Ø 100 mm specimen.

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B.J. Zhan, et al. Cement and Concrete Composites 104 (2019) 103360

Table 2
Curing and Conditioning and carbonation regimes adopted.
Samples Code Pre-conditioning Accelerated carbonation Further curing Total treating time

UnCarb (Reference) 25° ± 1 °C, 50 ± 1% RH, 7 days Nil 25° ± 1 °C, 50 ± 1%, 7 days 14 days
Carb_1d 100% CO2, +1 bar, 1 day 25° ± 1 °C, 50 ± 1%, 6 days 14 days
Carb_7d 100% CO2, +1 bar, 7 days Nil 14 day

treating time at 25 ± 1 °C and 50 ± 1% RH was 14 days. For the Eq. (1) to the acid-soluble Cl content of each layer:
Carb_1d samples, they were also cured at 25 ± 1 °C and 50 ± 1% RH
x
for 6 more days after the carbonation. It was to ensure the total treating C(x, t) = Cs − (Cs − Ci )erf ⎛⎜ ⎞
⎟
time for all the samples were 14 days for ease of comparison. ⎝ 4⋅ Da ⋅ t ⎠ (1)

where C(x, t) is the chloride concentration measured at depth x and

2.1.3. Test of transport properties
(1) Water absorption and sorptivity
The total amount of water absorbed and the rate of water absorption
(referred to as sorptivity) of the mortar attached to the RCA are im-
portant in assessing the water demand for concrete casting, as well as
the workability of RAC at the fresh state. In this study, triplicate cy-
linders (Ø 50 × 75 mm) obtained were used for determining the water
absorption according to the procedures given by BS EN 1097–6.
Sorptivity tests were carried out on three discs (Ø 100 × 50 mm)
after the accelerated carbonation treatment, in accordance with ASTM
C1585-13. After treatment, the discs were subjected to conditioning
regimes which were drying at a temperature of 50 ± 2 °C and RH of
80 ± 3% for 3 days, and then sealing in a container at 23 ± 2 °C for
15 days. Prior to the test, the circumference of each disc was sealed
with epoxy and the top end was covered with a plastic wrap to avoid
evaporation, leaving the sawn surface submerged in water. The sub-
sequent procedures for weighing the water uptake were conducted
according to ASTM C1585-13. The sorptivity was calculated by using
the increase in mass due to water uptake, divided by the cross-sectional
area of the specimen exposed to the water.
(2) Resistance of chloride penetration
Resistance of chloride ions penetration of the cement mortar was
assessed by the rapid chloride penetration (RCP) test (ASTM C 1202),
which was carried out on three Ø 100 × 50 mm discs. After the side
surface of the discs was sealed by a waterproof adhesive, then all
samples were vacuum saturated. During the test, two swan surfaces of
each specimen were exposed to sodium chloride solution (3% NaCl) and
sodium hydroxide solution (0.3 mol/L NaOH), respectively. A 60 V
external potential was applied and the current at 1 min intervals was
recorded for a 6 h period.
(3) Apparent chloride diffusion coefficient
In order to reveal the effect of accelerated carbonation treatment on
the chloride binding capacity of the cement mortars, the apparent
chloride diffusion coefficients of the mortar samples were determined
by measuring the acid-soluble chloride contents at different depths
from the surface exposed to the chloride solution. Two cylinders (Ø
50 × 75 mm) were selected for each measurement; all other sides of
cylinders were sealed with epoxy except the sawn surface which was
used as the exposed surface. After that, the procedures in ASTM C1556-
11a was followed to expose the specimen to a 16.5% NaCl solution at
25 ± 1 °C for 45 days. Powders were obtained by grinding off the
material in layers parallel to the exposed surface at 2 mm increments
until a depth of 20 mm was reached. Finally, the acid-soluble Cl content
in the powder of each layer was analyzed with a potentiometric titra-
tion method using silver nitrate (AgNO3) according with ASTM C1152.
The apparent chloride diffusion coefficient was determined by fitting
exposure time t in mass%, Cs is the chloride concentration at the in-
terface that is determined by the regression analysis in mass %, Ci is the
initial chloride concentration of the sample at time t = 0 in mass %, x is
the depth below the exposed surface in m, t is the exposure time in
seconds, Da is the apparent diffusion coefficient in m2/s, and erf denotes
the error function described in Eq. (2):
z
2
erf(z) =
π
∫ exp(−u2) du
0 (2)
(4) Bulk electrical conductivity
Measurement of bulk electrical conductivity was performed on three
discs (Ø 100 × 50 mm) according to the procedures described in ASTM
C1760-12, except that the thickness of the discs in this study was
50 mm. A thickness of 50 mm was expected to be sufficient to ensure
reliability of replicate test results due to the consistency in aggregate
content within the specimen with the maximum size of the aggregate
was smaller than 4.75 mm. This test measured the electrical current
through a saturated specimen with a potential (U) of 60 V DC across the
ends of the specimen. The current (I) was measured at 1 min after the
voltage was first applied. The electrical conductivity (σ, S/m) was
calculated by using Eq (3):
L I
σ= ⋅
A U (3)
with L, A as the disc length (0.05 m) and cross-sectional area
(0.00785 m2).
2.1.4. Thermogravimetric analysis
The content of calcium hydroxide (CH) and calcium carbonate (CC)
was measured as a function of the carbonation depth by using ther-
mogravimetric analysis (TGA). After grounding each layer described in
Section 2.3.3, the resulted powder samples were collected and dried in
an oven at 60 °C under vacuum for 48 h to remove the free water. The
temperature range for the TGA measurements (Rigaku, Thermo plus
EVO2) was 40–900 °C under a 10 mL/min flow of N2, with a constant
heating rate of 10 °C/min. According to the guidelines from Ref. [38],
the contents of CH and CC are calculated on the basis of Eqs. (4) and
(5):
CH = (74/18)∙(M450-M550)/M900 (4)
CC = (100/44)∙(M550-M900)/M900 (5)
where M is the weight at the subscripted temperature, the values of 74,
18, 44 and 100 g/mol are the molar mass of Ca(OH)2, H2O, CO2, and
CaCO3, respectively. Note that the temperatures indicated here are only
informative, the exact boundaries were determined based on the deri-
vative curves.
2.1.5. Scanning electron microscopy
The microstructural morphologies of the mortar samples were

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B.J. Zhan, et al. Cement and Concrete Composites 104 (2019) 103360

Table 3
Physical properties of RCA before and after carbonation.
Water absorption, Moisture Apparent density,
% content, % Kg/m3

Uncarbonated RCA 7.52 2.30 2636

Carbonated RCA 5.76 1.90 2700

analyzed by using a scanning electron microscopy (SEM, Tescan

VEGA3). The vacuum-oven dried strip specimen (20 × 7 × 3 mm3)
which was cut from the center part in the radial direction of the Ø
50 mm cylinder, was impregnated under vacuum with an epoxy resin
(EpoThin ™ 2), and gradually polished to 0.05 μm according to the
procedures described by Zhan et al. [18]. The well-polished surfaces of
Fig. 3. Schematic representation and dimensions (mm) of specimen for corro-
the samples were vacuum-dried again and then sputter-coated with a sion test.
conductive carbon layer using a SPI Module™ Carbon Coater. The BSE
images were acquired under a vacuum condition with a voltage of
15 kV and a working distance of 15.0 mm. Zhao et al. [39].

2.2. Steel corrosion in concrete incorporating carbonated RCA 3. Results and discussion

2.2.1. Materials and samples preparation
The RCA used in the current study was sourced from crushing a
batch of concrete with a known mix proportion produced by a local
concrete supplier [3,23], with the particle size ranging from 5 to
10 mm. Prior to the new concrete casting, the RCA was treated by ac-
celerated carbonation for 1 day using the procedures described for
Carb_1d in Table 2. The properties of RCAs before and after carbonation
treatment are listed in Table 3. Hot rolled steel round bars S275J0 (EN
10025–2: 2004) and stainless steel bars 304 L were used in the new
concrete (RAC) for the steel corrosion test.
Two groups of concrete were casted with uncarbonated RCAs (RAC)
and carbonated RCAs (CRAC) according to the mix proportions in
Table 4, respectively. Considering that uncarbonated RCA exhibited a
higher water absorption than the carbonated RCAs, the water demand
in the concrete mixtures was adjusted, to reach the consistent effective
water to cement ratio of 0.661, for both groups of RAC. The 28-d
compressive strength (fc) values of two groups RAC are also shown in
Table 4.
2.2.2. Set-up of steel corrosion test
For each group concrete, three cubic reinforced concrete specimens
with 100-mm length were cast for the steel corrosion test as shown in
Fig. 3. In each specimen, a 140-mm length hot rolled steel round bar
was used as a working electrode and another stainless steel bar served
as the auxiliary electrode.
2.2.3. Corrosion monitoring
After 35-days of curing, the prepared steel reinforced specimens
were subjected to a wet and dry cyclic condition (3 days wetting and
4 days drying) to speed up the corrosion process. During the wetting
period, the reinforced specimens were immersed in a 3.5% NaCl solu-
tion; while for the drying period, these specimens were taken out of the
solution and air dried in the laboratory at 25 °C. On the last day of each
cycle, the polarization curve of the working electrode was acquired by
using the electrochemical workstation (CorrTest CS350). Then the
Echem Analyst software was used, to determine the value of the po-
larization resistance Rp in accordance with the method described in
3.1. Results of transport properties of the carbonated mortar
3.1.1. Water transport properties
The water absorption and density results of the reference and the
carbonated mortar samples are presented in Fig. 4. The water absorp-
tion values decreased from 11.22% for the uncarbonated mortar to
8.97% for the 1d-carbonated mortar, and further decreased to 7.90%
for the 7d-carbonated mortar. While the density values increased from
1988 kg/m3 for the reference to 2105 kg/m3 for the 7d-carbonated
mortar. This behavior was consistent with our previous studies
[3,18,19].
In addition, the rate of water absorption or the sorptivity (S) of the
reference and carbonated mortar are also measured. Fig. 5 shows the
water uptake (water mass per unit inflow area) against square-root of
the elapsed time for the mortar samples. The typical standard deviation
of the mean values of the triplicate was less than 0.01 g/cm2 and it is
not shown here for clarity of the presentation. Comparing with the
reference mortar, the water absorption rate of the carbonated mortar
was lower. Extending the time of exposure to water induced a bigger
difference in water uptake. It can also be seen that the mortar samples
after 7-d of carbonation treatment has the lowest water absorption rate
during the whole testing process. The measured sorptivity, defined as
the slope of the curve shown in Fig. 5, was decreased by the carbona-
tion treatment. Therefore, the resistance to water infiltration of the
mortar can be enhanced by the accelerated carbonation treatment, and
this was consistent with an earlier study [26]. This is because after the
accelerated carbonation treatment, the hydrated cement matrix was
densified and the pores structure was refined due to the precipitation of
the formed calcium carbonates [40,41].

Table 4
Mix proportions and compressive strength of RAC.
Cement Water Fine aggregate RCA CRCA fc-28 (MPa)

RAC 310 244 723 997 / 28.4 ± 0.4

Fig. 4. Effects of accelerated carbonation treatment on water absorption and
CRAC 310 231 723 1010 31.9 ± 0.38
density of cement mortars.

4
B.J. Zhan, et al.
Fig. 5. Capillary water absorption of cement mortars after different treatment.
3.1.2. Chloride ions transport properties
The chloride ions transport properties were assessed in terms of the
total charge passed by RCPT and apparent chloride ions diffusion
coefficient. The total charge passed assessed by RCPT generally gives an
indirect estimate of the chloride resistance of the concrete. Although
the validity of the test is controversial, it is still widely used to assess the
chloride resistance of concrete in the concrete research community. The
experimental results of the mortar samples are shown in Fig. 6. The
current passed through the mortar specimen (Fig. 6(a)) indicate that the
current flow decreased obviously in the carbonated mortar specimen. It
is noteworthy that the current seemed to continuously increase until the
end of the test for the uncarbonated mortar, but tended to flatten out
after 3 h for the carbonated mortars. Fig. 6(b) shows that the total
charge passed for all the mortar samples reached over 4000 coulombs,
implying a high penetrability of Cl− ions. Nevertheless, when the data
show carbonation treatment induced a 18.2% decrease for the Carb_1d
mortar and 26.1% for the Carb_7d mortar.
Fig. 7 presents the profiles of total chloride concentration plotted
against the exposure depth of the mortar samples after 45 days of im-
mersion. Except the surface layer (up to a few mm) which has been
recognized as a convective zone [42], all the mortar samples showed a
typical decrease of total chloride content with increasing depth from
the exposed surface. The reference mortar shows the highest chloride
concentration from 4 mm, while the carbonated mortar samples ex-
hibited lower Cl− concentrations at all the depths than the reference.
The extended period of carbonation treatment also decreased the Cl−
concentration at the same depth in the mortar.
Based on the Cl concentration profiles at different depths, the ap-
parent chloride diffusion coefficients were determined by Eq (1), and
the results are shown in Table 5. Even subjecting to 1d carbonation
treatment, comparing with the reference, the Cl− diffusion coefficient
of the mortar was lowered by over 50%. But extending the treatment
Fig. 6. Results of the rapid chloride penetration test (RCPT): (a) evolution of current flow over time; (b) comparison of total charge passed of cement mortars.
5
Cement and Concrete Composites 104 (2019) 103360
Fig. 7. Chloride profiles measured at different depths in cement mortars.
Table 5
Apparent chloride diffusion coefficients of cement mortars determined after
exposure for 45 days.
Samples Code Fitted Cs (mass %) Da (10−12 m2/s) R-square
UnCarb 1.98 18.80 0.9301
Carb_1d 2.05 8.65 0.9747
Carb_7d 1.94 6.43 0.9573
time to 7 days only led to a slight further decrease in the diffusion
coefficient. This observation indicated that significant improvement of
resistance to the chloride ingress can be achieved by the accelerated
carbonation treatment. Ngala and Page also reported an enhanced re-
sistance to the Cl ions ingress in a plain cement paste after subjected to
carbonation [32]. This might be associated with the change of pore
structure induced by carbonation, while the capillary pores would be
partially filled through the deposition of calcium carbonate (CaCO3)
[25,28]. The details about pore profiles will be discussed in the fol-
lowing section. Moreover, carbonation reactions were reported to lead
to a decrease of the chloride binding capacity of cement pastes [43],
and thus it can be inferred that the underlying cause of the enhanced
resistance to the Cl ions ingress was mainly dominated by the pores
clogging induced by the carbonation reactions.
3.1.3. Bulk electrical conductivity
The electrical conductivity of cementitiuous materials reflects the
interconnectivity of pores network in the cement mortar, and thereby
gives a direct indication of the resistance to ionic transport. As there is a
good correlation between chloride diffusivity and electrical con-
ductivity of concrete [44], electrical conductivity is often used as a
quick tool for assessing the concrete quality. Fig. 8 depicts the bulk
B.J. Zhan, et al.
Fig. 8. Bulk conductivity of cement mortars.
electrical conductivity values of the mortar samples before and after the
accelerated carbonation treatment. After treatment by accelerated
carbonation for 1 day, the bulk electrical conductivity of the cement
mortar decreased from 2.51 × 10−2 S/m to 2.02 × 10−2 S/m.
(reduced by 19.6%), and further decreased to 1.75 × 10−2 S/m
(reduced by 30.3%) after subjecting to the accelerated carbonation
treatment for 7 days. Apparently, the result indicates that the ac-
celerated carbonation treatment had a significant influence on the bulk
electrical conductivity of the cement mortar. Many factors such as w/c
ratio, binders type, admixtures, and curing ages would affect the con-
ductivity of concrete [44]. However, for the current study, the carbo-
nation reactions in the cement mortar might be considered as the main
cause for the decrease of electrical conductivity, since carboantion
would alter the porosity, pore solution chemistry and tortuosity of the
pores network in the cement mortar [25,45].
3.1.4. Thermogravimetric analysis
Fig. 9 shows the contents of calcium carbonate (CC) and portlandite
(CH) determined by TGA in the ground sections of the mortar samples
as a function of the depth.
Due to the addition of limestone as a constitute for the manu-
facturing of cement, a small amount of CC (around 3%) were detected
in the reference samples (UnCarb). And little change of the contents of
CH and CC was found in the entire depth in the reference samples. In
the mortar samples subjected to the accelerated carbonation treatment,
the contents of CH and CC varied quite differently. Notably, there was a
signigicant increase in the CC content in the surface layer while a sharp
decline of CH content. The CC content at the surface layer reached up to
16.71% and varied little in the surface layer (< 5 mm) after 1-day of
carbonation treatment, and then sharply decreased for the depth >
5 mm, where the CH content gradually increased again. Both the
contents of CC and CH reached a relatively stable level at the depth
of > 12 mm. In the mortars subjected to carbonation treatment for 7
Fig. 9. Variation of portlandite (CH) and calcium carbonate (CC) contents with depth.
6
Cement and Concrete Composites 104 (2019) 103360
Fig. 10. SEM-BSE micrographs of mortar samples UnCarb, Carb_1d and Carb_7d
(left part) and binarization of the initial grey-level BSE images (right part). The
green zones of the binary image represent the pore areas. (For interpretation of
the references to colour in this figure legend, the reader is referred to the Web
version of this article.)
days, a similar trend can be observed. Extending the carbonation
treatment from 1 day to 7 days only resulted in a slightly increase of CC
content from 16.71% to 18.55% in the surface layer of the mortar. This
observation implys that the extended treatment seems not to be effec-
tive to further carbonate the samples. It might be due to lack of water
after the first 1 day of carbonation, together with the rising temperature
in the chamber due to the exothermic carbonation reaction driving
away the free water [43].
3.1.5. Microstructural observation
Fig. 10 shows BSE micrographs (left part) of the UnCarb, Carb_1d
and Carb_7d samples (from top to bottom), and their binarized images.
Clearly, the accelerated carbonation treatment resulted in variations of
the greyscale of the exposed surface layer. Quantitative analysis of
porosity was further carried out at different depths based on the method
proposed by Wong et al. [46], and the green zone in the right figures
represent the pore areas on the cross section. The details of the pore
profiles against the carbonation depth are shown in Fig. 11. Note that
the porosity here is a two-dimensional porosity corresponding to a re-
lative value. For the mortar samples not subjected to accelerated car-
bonation, the average porosity is around 20%, regardless of the sample
depth. After treatment by the accelerated carbonation for 1 day, the
porosity was markedly reduced at the surface layer (edge) of the
sample, then slowly increased until it reached the level of the un-
carbonated sample at the depth of 10 mm. Extended carbonation
treatment to 7 days could only further lower the porosity slightly, while
of the inner part (at the depth of 10 mm) reached the same value of the
uncarbonated sample. As highlighted in Section 3.1.4, the decrease of
porosity at the edge of the carbonated samples was mainly due to the
precipitation of calcium carbonates in the pores; this was also sup-
ported by the facts that the spatial gradient of the porosity is inversely
correlated with the CC content in the carbonated samples as shown in
B.J. Zhan, et al.
Fig. 11. Porosity profiles of mortar samples against depth.
Fig. 12. Polarization resistance of steels in RAC and CRAC over the drying and
wetting cycles.
Fig. 9.
3.2. Results of corrosion tests
Fig. 12 shows the polarization resistance (Rp) of RAC and CRAC over
the 12 drying and wetting cycles. It can be found that before the drying
and wetting cycles started, a higher Rp was observed in the RAC than
that in the CRAC. This is probably due to that the old cement mortar
attached on the RCA increased the alkalinity of the RAC. While the
alkalinity of CRCA decreased after the carbonation treatment, because
the carbonation treatment could reduce the free alkali metal and the
hydroxyl ions concentrations in the CRCA [45], and thus might also
lower the pH in the new concrete, which weakened the passivation of
the steel reinforcement, and decreased the chlorine ion threshold [47].
But, Rp of RAC decreased rapidly after the 11th drying and wetting
cycle. It meant that the steel embedded in RAC was corroded.
Meanwhile there was no obvious changes in Rp of CRAC over this
drying and wetting cycles, reflecting the steel in CRAC was still passi-
vated. This was because aggressive agents, such as Cl−, O2 and H2O,
were more accessible to the steel of the RAC prepared with un-
carbonated RCA, which initiated the corrosion of steel at an earlier
time. Meanwhile, the carbonation treatment enhanced the imperme-
ability of the old cement mortar adhered to the RCA [23], and to some
extent further improved the resistance to the penetration of deleterious
species into the concrete. Therefore, it has been demonstrated that the
carbonation modification of RCA improved the protection of steel from
corrosion. Moreover, the improvement of the new interfacial transition
zone (ITZ) around the RCA caused by carbonation may also partially
contribute to the improvements in resisting the penetration of water
7
Cement and Concrete Composites 104 (2019) 103360
and chloride ions [23]. Future studies are being carried out by the
authors to quantify the effects of the carbonation treatment of RCA on
the properties of ITZ in new concrete.
4. Conclusions
The old attached mortar on the RCA seriously affect the durability of
the RAC, and revealing the variation of the transport properties of ce-
ment mortars subjected to accelerated carbonation treatment is crucial
with respect to understanding the effects of carbonated RCA on the
durability of RAC.
Based on the results of the water and Cl ions transport tests, it was
evident that the water absorption and sorptivity, total charge passed
and Cl ions diffusion coefficient, as well as the bulk electrical con-
ductivity of the cement mortar was decreased after the mortar samples
were subjected to the accelerated carbonation treatment. Extending the
carbonation treatment from 1 day to 7 days only resulted in a marginal
decrease of the transport properties. A significant decrease in porosity
at the surface layer of the cement mortar determined by SEM-BSE was
observed, agreeing well with the high CC contents found in the surface
layer by using TGA. The spatial gradient of porosity and CC/CH con-
tents illustrated that even only with the external layer (0–10 mm) car-
bonated, a considerable improvement of transport properties of the
cement mortar could still be achieved. The corrosion test of the steel bar
in the new RAC concrete also confirmed that the corrosion resistance of
steel bar in the RAC can be improved by incorporating the carbonated
RCA.
Acknowledgement
The authors wish to thank the Hong Kong Research Grants Council
Poly U152144/17E and The Hong Kong Polytechnic University for
funding supports.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.cemconcomp.2019.103360.
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