Construction and Building Materials 154 (2017) 810–818

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Construction and Building Materials

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

Effect of CO2 curing on demolition recycled fine aggregates enhanced by

calcium hydroxide pre-soaking
Ganghua Pan a,b,⇑, Mimi Zhan a,b, Minghua Fu a,b, Yaping Wang a,b, Xiaojun Lu c
a
School of Materials Science and Engineering, Southeast University, Nanjing 211189, PR China
b
Jiangsu Key Lab of Construction Material, Southeast University, Nanjing 211189, PR China
c
Jiangsu Zhenjiang Research Institute of Building Science Group Co., Ltd, Zhenjiang 212004, PR China

h i g h l i g h t s

Pre-soaking process improved CO2 curing efficiency on recycled fine aggregate (RFA).

CO2 cured RFA showed low water absorption, powder content and crush value.

Mortars with carbonated RFA achieved excellent flowability and high strength.

CaCO3 from carbonation reaction reduced the porosity of RFA and relative mortars.

a r t i c l e i n f o a b s t r a c t

Article history: Because of a long storage time, recycled fine aggregates (RFAs) derived from demolition concrete have an
Received 24 June 2016 extremely low content of carbonatable compounds, which makes it difficult to improve their perfor-
Received in revised form 13 March 2017 mance through a regular carbonation process. In this study, we attempted to increase the content of car-
Accepted 6 July 2017
bonatable compounds in demolition RFAs via calcium hydroxide (CH) pre-soaking for enhancing the
Available online 17 August 2017
carbonation effectiveness. RFAs pre-soaked with CH before carbonation exhibited better properties,
including a lower crush value, water absorption, and powder content, as well as a higher strength, than
Keywords:
RFAs subjected to carbonation alone. The effect of the carbonation parameters on CO2 curing was exam-
Recycled fine aggregate (RFA)
CO2 curing
ined, and the optimal condition was identified. Experimental results show that the crush value, water
Calcium hydroxide absorption, and powder content were significantly reduced by curing the RFAs under the optimal condi-
Water absorption tion (ORFAs). Moreover, the flowability of mortars prepared with ORFAs was improved, and the compres-
Compressive strength sive strength at 28 d was increased. The porosity of mortars made prepared using ORFAs was reduced,
and the pore structure was refined, as revealed by a mercury intrusion porosity test. The enhancement
mechanism was investigated using X-ray diffraction and scanning electron microscopy.
Ó 2017 Elsevier Ltd. All rights reserved.

1. Introduction
Recently, the annual increase in construction demolition waste
has been burdensome for the environment [1–5]. The reuse of con-
struction waste is imperative for saving natural resources, protect-
ing the environment, and achieving sustainable development in
the construction industry [6]. However, the poor quality of recy-
cled aggregates (RAs), including their high water absorption and
low strength, hinders their application in the construction industry
[2,7]. Many pretreatments for minimizing these adverse effects
have been developed, and the methods used to compensate for
⇑ Corresponding author at: School of Materials Science and Engineering,
Southeast University, Nanjing 211189, PR China.
E-mail address: 101004929@seu.edu.cn (G. Pan).
the poor quality of RAs can be classified into two categories: (1)
removing the attached mortar of the RAs via ultrasonic cleaning
[8], ball milling [9], heating etc. and then rubbing or pre-soaking
the RAs with an acid solution (HCl, H2SO4, or H3PO4) [10]; and
(2) improving the quality of the attached old cement paste by cov-
ering the surface with water glass (Na2OnSiO2) [1,7], pozzolanic
materials [1], or a polymer solution such as a polyvinyl alcohol
emulsion [11]. However, pre-soaking RAs with acidic solutions
often introduces acid ions into the RAs, thereby decreasing the
pH of the cement products. Polymer solutions effectively reduce
the water absorption of RAs but cause a limited increase in
strength. In addition, the RAs must be sieved before the aforemen-
tioned pretreatment methods, which increases the complexity and
cost of these processes and reduces the utilization of RAs.

http://dx.doi.org/10.1016/j.conbuildmat.2017.07.079
0950-0618/Ó 2017 Elsevier Ltd. All rights reserved.
 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
Carbonation is an alternative method for improving the surface
hardness, strength, and durability of cement products by altering
the pore refinement of the cement paste [12–15]. Moreover, the
CO2 absorption process used to enhance the properties of RAs
should be considered in environmental assessments aimed at
reducing CO2 emissions, in accordance with the goal of achieving
sustainable development in the construction industry [1,16–18].
The idea of exploiting carbonation has been proposed [19–25], par-
ticularly for non-reinforced cement-based composites. However,
most research to date has focused on the CO2 curing of concrete
containing natural aggregates. Few studies involved the use a
CO2 curing technique for improving the properties of RAs. Zhan
et al. [26] reported that after a carbonation process, the density
and 10% fine value of RAs had increased, and the water absorption
was significantly reduced. Xiao et al. [27] suggested that at a high
water-to-binder ratio (w/b), the carbonation effect is more obvi-
ous. Kou et al. [28] reported that concrete prepared with RAs cured
in a 100% CO2 chamber under a pressure of 0.1 bar exhibited high
density and low water absorption. Shi et al. [29] reported that CO2
curing significantly decreased the crushing value and water
absorption of RAs and slightly increased the apparent density of
the RAs.
However, the RAs used in the aforementioned studies [26–29]
were mostly obtained from crushed concrete prepared in a labo-
ratory, which had enough carbonatable compounds to achieve an
ideal carbonation curing result. Normally, there are not enough
carbonatable compounds in RAs sourced from demolished con-
crete pieces, because of long-term storage; thus, these RAs do
not exhibit the same carbonation effect as the RAs produced in
a laboratory. To solve this problem, CH pretreatment was per-
formed before the carbonation process. The curing process was
conducted under atmospheric pressure. To our knowledge, this
is the first application of the proposed technique. The optimal
CH concentration and CO2 curing condition were determined,
and the effects of CO2 curing on the physical and mechanical
properties of the RFAs were examined. The effects of the CO2 cur-
ing technique on the properties of fresh and hardened mortars
were also investigated.
2. Materials and experiments
2.1. Materials and characteristics
2.1.1. Aggregates
Natural river sand and demolition concrete waste (supplied by the Jiangsu
Zhenjiang Research Institute of Building Science Group Co., Ltd.) were used as nat-
ural fine aggregates (NFAs) and RFAs. The demolition concrete wastes, which had
been stored for 1 year, were subjected to a primary crushing procedure and then
indoors, where they were kept under natural conditions. The physical properties
and surface micromorphology of the fine aggregates are given in Table 1 and
Fig. 1, respectively. SS in Table 1 represents standard sand. Compared with the
NFAs, the RFAs had a higher crush value, water-absorption value, and powder con-
tent. The surface of the NFAs was smooth, with only a few shallow pores, whereas
the surface of the RFAs was relatively rough, with clear microcracks. These results
indicate the poor quality of the RFAs.
To prove the necessity of CH addition, the content of carbonatable compounds
(mainly CH) was examined using thermogravimetric (TG) analysis before CO2 cur-
ing. As shown in Fig. 2, the mass loss of CH in the RFAs was extremely low (only
1.57%), whereas the content of CaCO3 was as high as 9.32%. According to literature
[29], there were still CH residues (1.81%) in the RFAs, even if they underwent a com-
plete carbonation process, which means that the CH in the RFAs was not completely
Table 1
Physical properties of aggregates.
Aggregate type Fineness modulus Powder content (<0.15 mm)/%
NFA 2.7 2.0
RFA 2.8 14.2
SS 3.0–2.3 9.56
811
carbonated to CaCO3 via a regular process. Thus, it may be concluded that the CH
content that was carbonated in this study was less than 1.57% without any
pretreatment.
2.1.2. Cementitious material
The cement used was P.O42.5 and was produced in the Jiangsu Helin Cement
Plant. Type II grade fly ash was obtained from the Zhenjiang Jianbi Power Plant.
Thickening powder was supplied by the Jiangsu Zhenjiang Research Institute of
Building Science Group Co., Ltd.
2.1.3. Calcium hydroxide
Owing to the low content of carbonatable compounds in the demolished RFAs,
CH solutions were used to pre-soak the RFAs before CO2 curing. The CH used in this
study was supplied by the Xilong Chemical Company.
2.2. Experimental program
2.2.1. CH pretreatment
A CH solution was used to pre-soak the RFAs for increasing the content of car-
bonatable compounds. The RFAs were placed in a container, immersed in the CH
solution, and steadily stirred to ensure that their surface remained moist for 24 h.
Then, the pretreated RFAs were dried in an oven at 105 °C until their moisture con-
tent satisfied the experimental requirements (see Table 2). CH solutions with differ-
ent concentrations, given in Table 2, were employed to evaluate the effects of the
CH concentration on the curing process.
2.2.2. CO2 curing process
After a pre-soaking and drying process, the RFAs were placed in a carbonation
chamber (Fig. 3) at a temperature of 20 ± 2 °C and a relative humidity of 60 ± 5%
for CO2 curing. Commercially supplied CO2 with a purity of 99.5% was used for
the CO2 curing experiment. To examine the influence of various curing regimes
on the properties of the RFAs, several parameters were varied and tested during
the CO2 curing process. The variables tested, including the CO2 concentration
(CO  
2 ), moisture content of the RFAs (M ), and CH concentration (CH ), are detailed
in Table 2. All the experiments were performed under atmospheric pressure. The
RFAs in batch CO 2 were cured with a CO2 concentration ranging from 20% to
100%. For the CH batch, CH solutions in the concentration range 0.01–0.25-mol/
kg were prepared for pre-soaking the RFAs. RFAs that did not undergo CH pre-
soaking were also placed in the curing chamber as a reference. The M batch was
examined as the moisture content was increased from 2.5% to 7.5%.
The moisture content of the RFAs was controlled according to methods given in
literature [30]. The specific operational steps were as follows. First, the RFAs sam-
ples were oven-dried to obtain a constant mass value M0. Second, the oven-dried
samples were uniformly immersed with water or CH solutions for 24 h. Third, the
samples were dried in an oven to remove some of the water. The water loss of
the samples was monitored during the drying process, and the moisture content
(w) of the samples was determined using the following equation:
w ¼ ðMi  M0 Þ=ðM0 Þ  100%; ð1Þ
where M0 represents the mass of the RFA samples oven-dried to a constant value,
and Mi represents the mass of the sample after the drying process. For each batch,
the curing process was continued until a phenolphthalein indicator revealed no col-
oration in the RFAs.
2.2.3. Preparation of mortar mixtures
Masonry mortars with a compressive-strength grade of 10 MPa were prepared,
and the mix proportions are provided in Table 3. During the preparation process,
the consistency was controlled between 70 and 90 mm by adjusting the water con-
sumption. The aggregates used in the mortar preparation were in an oven-dried
condition. The mortar mixes were cast in 40  40  160-mm3 plastic molds, com-
pacted using a vibrating table, covered with a plastic sheet, and then cured in the
laboratory. The specimens were demolded after 24 h and further cured in a water
curing tank at 27 ± 1 °C for 28 d. At 28 d, all the specimens were removed from
the curing tank for various tests.
Apparent density (kg/m3) Water absorption at 24 h/% Crush value/%
2600 1.19 16
2640 4.35 18
2610 0.26 7.15
812 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
Fig. 1. Scanning electron microscopy (SEM) images of fine aggregates: (a) natural river sand and (b) demolition RFAs.
Fig. 2. TG curve of RFA (particle size < 4.75 mm).
2.3. Testing
Tests were performed investigate the physical and mechanical properties of the
RFAs and the corresponding mortars. The properties of the RFAs were determined in
accordance with Chinese standards GB/T25176-2010 [31] and GB/T14684-2011
[32], including the crush value, water absorption, powder content, water-demand
ratio of the recycled mortar, and compressive-strength ratio of the recycled mortar.
The water-demand ratio of recycled mortar is defined as the ratio of the water
volume needed for the recycled mortar with 130 ± 5 mm fluidity to that needed for
reference mortar with 130 ± 5 mm fluidity, which made of SS. The compressive-
strength ratio is defined as the ratio of the compressive strength of the recycled
mortar with 130 ± 5 mm fluidity to the reference mortar with 130 ± 5 mm fluidity,
which is made of SS and aged for 28 d. All the procedures were conducted under the
guidance of the Chinese standard GB/T25176-2010 [31]. Additionally, the tests
of the corresponding mortars were conducted in accordance with the Chinese
standards GB/T25181-2010 [33] and JGJ/T70 [34], including the water/binder ratio,
consistency loss, apparent density, setting time, and water retention. The water
retention was assessed by using the procedure of JGJ/T70 [34] and calculated
according to the water content of the mortar samples before and after suction by
filter paper.
The microstructure of the specimens was observed using a field-emission scan-
ning electron microscope (Sirion 20042136). X-ray diffraction (XRD) data were col-
lected using a D8 Advance instrument from Bruker AXS. TG analysis was performed
using a TherMax 500 Thermal Analyzer. A dry sample of approximately 50 mg was
heated at a rate of 10 °C/min in a nitrogen atmosphere from 50 to 1000 °C. The
pore-size distribution was evaluated using mercury intrusion porosity (MIP).
Table 2
Details regarding the CO2 curing regime.
Batch Aggregate abbreviation CO2 concentration/%
CO2- CO2-20/50/70/100 20/50/70/100
M- M-2.5/5/7.5 70
CH- CH-0/0.01/0.05/0.25 70
3. Results and discussions
3.1. Aggregates
3.1.1. CH pretreatment
Fig. 4(a) shows the particle grading curves of the RFAs in the
CH- batch. The effects of CH concentration on the properties of
the RFAs are illustrated in Fig. 4(b) and Table 4. The values are
the averages of three measurements.
CH-0 represents the RFAs carbonated without CH pretreatment.
As observed in Table 4, without CH pre-soaking, the properties of
CH-0 improved negligibly after CO2 curing, indicated by a 1% incre-
ment in the crush value and a <1% decrease in water absorption
and powder content. However, CH pretreatment before CO2 curing
caused a noticeable improvement in the properties of the RFAs, as
indicated by the significant reduction of the crush value, water
absorption, and powder content. This result occurred because the
addition of CH facilitated the formation of CaCO3 during the curing
process. The produced CaCO3 had a twofold impact on the RFAs: (1)
a micro-packing effect that optimized the pore structures, which
reduced the crush value and water absorption; and (2) a covering
effect that increased the powder size, which reduced the powder
content to <0.15 mm. More importantly, the water-demand ratio
of RFAs treated with CH decreased and the compressive-strength
ratio increased, whereas CH-0 did not exhibit an obvious improve-
ment in the water-demand ratio and compressive-strength ratio.
The above results indicate that the regular carbonation process
without CH pretreatment cannot significantly improve the proper-
ties of demolished RFAs, owing to the low content of carbonatable
compounds. Thus, CH pretreatment is considered as a beneficial
procedure for improving the carbonation effects on demolished
RFAs.
When CH concentration increased from 0.01 to 0.25, the crush
value increased from 13% to 16%, the water absorption increased
from 1.65% to 2.35%, the powder content decreased from 9.1% to
8.8%, and the water-demand ratio increased from 1.10 to 1.17. This
suggests that a higher CH concentration did not cause a better car-
bonation effect. Two factors may have contributed to this phe-
nomenon: (1) an insufficient amount of CO2 penetrated the RFAs
to react with all the free Ca2+ ions in the pore solution; (2) the RFAs
became denser after carbonation, which hindered the further infil-
tration of CO2 into them. However, unlike the water absorption,
Moisture content of RFA/% CH treatment /(mol/kg)
0.2 0.01
2.5/5/7.5 0.01
5 0/0.01/0.05/0.25
 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818 813

Fig. 3. Schematic of the CO2 curing setup.

Table 3
Mix proportions of mortars.

Mortar type Cement/g FA/g Thickening powder/g Replacement level/% River Sand/g RFA/g
M-NFA 240 60 20 0 1500 0
M-RFA 240 60 20 100 0 1500

Fig. 4. (a) Particle grading curves of RFAs and (b) the effects of CH concentration on the water-demand ratio and compressive-strength ratio of recycled mortar.

Table 4
Effects of CH concentration on the physical properties of the RFAs.

Aggregate type CH concentration (mol/kg) Crush value/% Water absorption/% Powder content (particle size < 0.15 mm)/%
RFA – 18 4.35 14.2
CH-0 0 19 3.75 13.8
CH-0.01 0.01 13 1.65 9.1
CH-0.05 0.05 14 2.00 9.0
CH-0.25 0.25 16 2.35 8.8

crush value, and water-demand ratio, the compressive-strength
ratio of the recycled mortar was enhanced when CH concentration
increased from 0.01 to 0.25. This indicates that other factors
affected the compressive-strength ratio. The aforementioned
results suggest that a very high CH concentration is not desirable
and that a moderate CH concentration is sufficient for improving
the properties of RFAs.
3.1.2. CO2 concentration
Table 5 presents the effects of the CO2 concentration on the
physical properties of the RFAs. The values shown are the averages
of three measurements. Clearly, the CO2 curing enhanced the phys-
ical properties of the RFAs, as indicated by the lower crush value,
water absorption, and powder content. This is because the CaCO3
generated by the reaction between CO2 and the hydration products
814 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
Table 5
Physical properties of RFAs carbonated at different CO2 concentrations.
Aggregate type CO2 concentration/% Crush value/%
RFA – 18
CO2-20 20 10
CO2-50 50 12
CO2-70 70 13
CO2-100 100 15.8
filled the pores and microcracks in the RFAs [29]. When the CO2
concentration increased from 20% to 70%, the water absorption
gradually decreased from 2.00% to 1.65%, and then returned to
2.00% at 100% CO2. However, the crush value continued to increase
(from 10% to 15.8%) as the CO2 concentration increased from 20%
to 100%. This unexpected result is ascribed to the reduction in
the powder content (from 14.0% to 5.26%) at a high CO2 concentra-
tion. The filling effect of the powder can lead to a low crush value;
thus, the reduction in the powder content resulted in a high crush
value. There was no further improvement in the crush value and
water absorption as the CO2 concentration increased to 100%.
There are two reasons for these results: (1) the denser surface of
the RFAs caused by carbonation reduced the rate of CO2 diffusion
into the RFAs [35]; (2) the high CO2 concentration allowed a large
amount of CO2 to react with calcium–silicate–hydrate (CSH) to
form a phase with a lower Ca/Si-ratio, thereby increasing the
degree of decalcification of CSH [36]. Similar to the water absorp-
tion, the water-demand ratio of the RFAs steadily decreased as the
CO2 concentration increased from 20% to 70%, and then increased
to 1.14 at 100% CO2. The compressive-strength ratio increased
slightly (from 0.97 to 1.04) as the CO2 concentration increased
from 20% to 70%, and then decreased to 0.99 at 100% CO2. This
may be related to the inferior physical properties of the RFAs cured
at 100% CO2. The RFAs cured at 70% CO2 exhibited a lower water-
demand ratio and the highest strength ratio among the four
batches tested. Thus, we infer that 70% is the optimal CO2 concen-
tration for improving the properties of RFAs via curing.
3.1.3. Moisture content of aggregates
Batch M was designed to study the influence of the moisture
content of the RFAs on the effectiveness of carbonation. The RFAs
in batch M were pretreated with 0.01 mol/kg CH and then cured
in the chamber at 70% CO2. The averages of the three experimental
results are presented in Fig. 6.
As shown in Fig. 6(a), after the curing process, the intrinsic
problem of RFAs—high water absorption—was improved. The
Fig. 5. Water-demand ratio and compressive-strength ratio of recycled mortar
carbonated at different CO2 concentrations.
Water absorption/% Powder content (particle size < 0.15 mm)/%
4.35 14.2
2.00 14.0
1.23 10.5
1.65 9.7
2.00 5.26
water absorption decreased from 1.93% to 1.65% when the mois-
ture content increased from 2.5% to 5% and then increased to
2.95% at a moisture content of 7.5%. Thus, the sustained increase
in the moisture content cannot lead to a sustained improvement
in water absorption. The porosity exhibited the same trend, as
shown in Fig. 6(b). The porosity of the cured RFAs decreased from
6.01% to 3.66% as the moisture content increased from 2.5% to 5%
and reached its minimum value at a moisture content of 5%. Fur-
ther increase in the moisture content did not decrease the porosity.
However, the cured RFAs all had a lower porosity than pristine
RFAs. The variation in water absorption and porosity is attributed
to the complex effect of moisture content on CO2 diffusion. Below
the optimal moisture content, the matrix was too dry, and there
was not much water for the carbonation reaction to occur. How-
ever, above the optimal value, the saturation of pores with water
hindered the diffusion of CO2, which had an adverse impact on
the carbonation rate [30].
The experimental results for the water-demand ratio and the
compressive-strength ratio of the RFAs with different moisture
contents are illustrated in Fig. 6(c). After CO2 curing, the water-
demand ratio and compressive-strength ratio of the RFAs varied
within the narrow ranges of 1.15–1.10 and 0.97–1.04, respectively.
The M-5 batch, which was cured at a moisture content of 5%,
exhibited the lowest water-demand volume and the highest
strength. The compressive-strength ratio of the M-5 batch was
even higher than that of standard sand. The trends of the water-
demand ratio and compressive-strength ratio with respect to the
moisture content are similar to those of the water absorption
and porosity. This suggests that the moisture content of the aggre-
gates is a critical factor that influences the carbonation reaction
rate. Too much or too little moisture is unfavorable for the diffu-
sion of CO2, which is consistent with the results obtained by Zhan
et al. [30]. In this study, a moisture content of 5% was the optimal
value.
3.1.4. XRD analysis of RFAs
To further investigate the enhancement mechanism of carbon-
ation, the RFAs were pre-soaked in a 0.01-mol/kg CH solution
and then cured under the optimal condition—70% CO2 and a mois-
ture content of 5%—and labeled as ORFAs. The XRD patterns of the
RFA and ORFA are shown in Fig. 7. CaCO3 was detected in the ref-
erence RFA and ORFA. A comparison between the XRD patterns of
the RFA and the ORFA reveals that the content of CaCO3 in the
ORFA was increased. This increase likely resulted from the carbon-
ation process. The CaCO3 in the ORFA mainly existed in the form of
calcite. The CaCO3 produced by the carbonation process filled the
pores and microcracks in the RFAs, improving their properties.
3.1.5. SEM images
To investigate the microstructure of the cured RFAs, scanning
electron microscopy (SEM) images were obtained. Fig. 8 shows
the SEM images of RFAs cured at different CO2 concentrations.
CaCO3—the main product of the carbonation reaction—is repre-
sented by the red arrow. Fig. 8 shows that the CaCO3 produced
by carbonation mainly appears as irregular granules. The size of
the CaCO3 formed in the CO2-20 batch was approximately
 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
Fig. 6. Effects of moisture content on the properties of the RFAs: (a) water absorption, (b) porosity, (c) water-demand and compressive-strength ratios of recycled mortar.
Fig. 7. XRD patterns of the RFA and ORFA.
5–10 lm, whereas the CaCO3 in the CO2-50 batch was smaller:
3–5 lm. These effects may be related to the higher concentration
of CO2 used in the CO2-50 batch. However, when the concentration
of CO2 increased to 70% and 100%, the size of the CaCO3 particles
remained at 3–5 lm. Because of a better filling effect, the smaller
CaCO3 particles were more beneficial for improving the properties
of RFAs. Thus, RFAs cured at a higher CO2 concentration may
exhibit better properties.
3.2. Mortars
3.2.1. Physical and mechanical properties of mortars
Mortar specimens made with NFAs and 100% pristine RFAs
were prepared for reference. Mortar specimens made with 100%
RFAs and cured under optimal conditions were labeled as
815
M-ORFA. The mix proportions and physical properties are
presented in Tables 3 and 6. The values are the averages of three
measurements. Table 6 shows that for the mortars made with
cured RFAs, the consistency loss and w/b ratio were both low
because of the low water absorption. Furthermore, the consistency
loss of the M-ORFA samples was even smaller than that of the
M-NFA. As expected, the setting time for the M-ORFA was longer
than that of the M-RFA. This is because the decreased consistency
loss and high water-retention capacity allowed the material to
hold a large amount of free water during the mortar preparation.
Additional free water in the matrix caused the cement particles
to be farther apart, which increased the time required for the
matrix to be set. Interestingly, the reference mortar specimen
made with uncured RFAs exhibited the highest apparent density,
even higher than that of the M-NFA. The apparent density of the
M-ORFA was higher than that of the M-NFA but was lower than
that of the M-RFA. This behavior might be related to the high water
retention (89.8%) of the M-RFA, which created an internal curing
environment in the cement matrix.
Fig. 9 presents the compressive strengths of the mortar speci-
mens made with NFAs, pristine RFAs, and ORFAs at 28 d. Clearly,
both M-RFA and M-ORFA had a higher compressive strength
(13.8 and 14.0 MPa, respectively) than M-NFA (11.1 MPa). This is
because the higher water retention of M-RFA and M-ORFA pro-
vided an internal curing environment, increasing compressive
strength during the 28-d curing period. However, the M-ORFA
specimen achieved a slightly higher compressive strength than
the M-RFA specimen, even though M-RFA had the highest water
retention (see Table 7). This is ascribed to the enhanced physical
properties of M-ORFA. The results suggest that the carbonation
process facilitated the improvement of not only the properties of
the RFAs but also the mechanical properties of the corresponding
mortars.
816 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818

Fig. 8. SEM images of (a) CO2-20, (b) CO2-50, (c) CO2-70, and (d) CO2-100.

Table 6
Properties of the mortars.

Notation Water/binder ratio Consistency loss/mm Consistency loss ratio at 2 h/% Water retention/% Apparent density/(kg/m3) Setting time/min
M-NFA 0.83 78 28.9 84.5 1830 505
M-RFA 1.03 75 50.0 89.8 1890 336
M-ORFA 0.90 73 28.8 89.4 1840 360

3.2.2. Porosity of mortars

Fig. 9. Compressive strength of mortar mixtures at 28 d.
To further study the improvement mechanism of the carbona-
tion process, the porosity of mortars was measured, and the results
are presented in Table 7 and Fig. 10. According to Silva [37], Jen-
nings [38], Mehta and Monteiro [39], the pores listed in Table 7
were classified into the following categories: macro and entrained
air pores (>1 lm), large capillary pores (50 nm–1 lm), medium
capillary pores (10–50 nm), and gel pores (<10 nm). Surprisingly,
the mortars prepared with uncured RFAs exhibited a lower total
porosity than those prepared with NFAs. This phenomenon is
attributed to two factors: (1) the RFAs were carbonated to some
extent during storage; (2) there were far more capillary pores in
the M-NFA. As expected, the mortars made with ORFAs exhibited
the lowest porosity. Moreover, the macro and entrained air poros-
ity of the M-ORFA was noticeably reduced, and the medium capil-
lary porosity was significantly increased. This demonstrates that
the pore structure of the M-ORFA was substantially refined by
the carbonation product CaCO3.

Table 7
Porosity of the mortar mixtures.

Mortar type Total porosity/% Medium capillary porosity Large capillary porosity Macro porosity and entrained
(10–50 nm)/% (50 nm–1 lm)/% air porosity (>1 lm)/%
M-NFA 34.89 7.93 7.52 5.08
M-RFA 29.95 6.45 7.46 9.62
M-ORFA 28.46 8.46 7.37 5.16
 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
Fig. 10. (a) Pore-size distribution and (b) cumulative pore volume.
Fig. 10(b) shows the characteristic curves of the volume of
intruded mercury with respect to the pore radius of the mortars.
There are at least three major peaks in the pore-size distribution
curves of the mortar samples. The first ranges from approximately
5–100 nm; the second, which is the sharpest, ranges from 100–
4  103 nm; and the third ranges from 10 to 100 lm. According
to the refinement phenomenon observed in Table 7, the second-
peak value for M-ORFA was lower than those for M-NRA and
M-RFA. In the small pore-size range, the first-peak value for the
M-ORFA was higher than that for the M-RFA. This behavior is
associated with the filling and refinement effect of the CaCO3
formed during the carbonation reaction. These results confirm that
the CH pretreatment combined with CO2 curing improved the
properties of the RA mortars.
4. Conclusions
Based on the tests conducted during this study, the following
conclusions can be drawn:
(1) CH pretreatment is beneficial for improving the properties of
RFAs derived from demolition concrete after a long storage
time. By comparing the properties of RFAs cured under var-
ious conditions, the optimal CO2 curing condition was iden-
tified as follows: a 0.01–0.05-mol/kg CH solution, CO2
concentration of 70%, and moisture content of 5%.
(2) After the CO2 curing process, the powder content of the RFAs
decreased from 14.2% to 9.1%, the water absorption
decreased from 4.35% to 1.65%, and the crush value
decreased from 18% to 13%. In addition, the water-demand
ratio of the cured RFAs decreased from 1.17 to 1.10,
and the compressive-strength ratio increased from 0.95 to
1.04.
(3) Compared to the mortar made with pristine RFAs, the mor-
tar made with cured RFAs exhibited better flowability,
including a lower w/b ratio and consistency-loss value and
a longer setting time. Moreover, the compressive strength
of the mortar made with cured RFAs was approximately
26% higher than that of the mortar made with NFAs after
28 d.
(4) XRD patterns and SEM images revealed that the curing pro-
cess generated CaCO3 via carbonation reactions. Because the
generated CaCO3 filled the pores of the RFAs, the porosity of
the RFAs and the corresponding mortars were reduced, and
the pore structure of the mortars was refined, as indicated
by the MIP tests.
817
Acknowledgements
This research did not receive any specific grant from funding
agencies in the public, commercial, or not-for-profit sectors.
References
[1] J. Li, H. Xiao, Y. Zhou, Influence of coating recycled aggregate surface with
pozzolanic powder on properties of recycled aggregate concrete, Constr. Build.
Mater. 23 (3) (2009) 1287–1291.
[2] Q. Liu, J. Xiao, Z. Sun, Experimental study on the failure mechanism of recycled
concrete, Cem. Concr. Res. 41 (10) (2011) 1050–1057.
[3] P.S. Lovato, E. Possan, D.C.C. Dal Molin, Â.B. Masuero, J.L.D. Ribeiro, Modeling of
mechanical properties and durability of recycled aggregate concretes, Constr.
Build. Mater. 26 (1) (2012) 437–447.
[4] J. Sim, C. Park, Compressive strength and resistance to chloride ion
penetration and carbonation of recycled aggregate concrete with varying
amount of fly ash and fine recycled aggregate, Waste Manage. 31 (11) (2011)
2352–2360.
[5] F.P. Torgal, S. Miraldo, J. Labrincha, J. De Brito, An overview on concrete
carbonation in the context of eco-efficient construction: evaluation, use of
SCMs and/or RAC, Constr. Build. Mater. 36 (2012) 141–150.
[6] J. Qiu, D.Q.S. Tng, E.-H. Yang, Surface treatment of recycled concrete aggregates
through microbial carbonate precipitation, Constr. Build. Mater. 57 (2014)
144–150.
[7] H. Cheng, C. Wang, Experimental study on strengthen concrete regenerated
aggregate with water glass, New Build. Mater. 12 (2004) 12–14.
[8] A. Katz, Treatments for the improvement of recycled aggregate, J. Mater. Civil.
Eng. 16 (6) (2004) 597–603.
[9] D. Montgomery, Workability and compressive strength properties of concrete
containing recycled concrete aggregate, sustainable construction: use of
recycled concrete aggregate, in: Proceedings of the International Symposium
by the Concrete Technology Unit, University of Dundee, UK on, 1998, pp. 287–
296.
[10] V.W. Tam, C. Tam, K.N. Le, Removal of cement mortar remains from recycled
aggregate using pre-soaking approaches, Resour. Conserv. Recycl. 50 (1)
(2007) 82–101.
[11] S.C. Kou, C.S. Poon, Properties of concrete prepared with PVA-impregnated
recycled concrete aggregates, Cem. Concr. Compos. 32 (8) (2010) 649–654.
[12] J. Han, G. Pan, W. Sun, C. Wang, D. Cui, Application of nanoindentation to
investigate chemomechanical properties change of cement paste in the
carbonation reaction, Sci. China. Technol. Sci. 55 (3) (2012) 616–622.
[13] G. Pan, C. Wang, H. Rong, Application of X-ray computed tomography in
characterization microstructure changes of cement pastes in carbonation
process, J. Wuhan. Univ. Technol. Sci. 27 (2) (2012) 358–363.
[14] J. Han, W. Sun, G. Pan, W. Caihui, Monitoring the evolution of accelerated
carbonation of hardened cement pastes by X-Ray computed tomography, J.
Mater. Civil. Eng. 25 (3) (2012) 347–354.
[15] J. Han, G. Pan, W. Sun, Elastic modulus change investigation of cement paste
before and after carbonation using nanoindentation technique, Procedia Eng.
27 (2012) 341–347.
[16] R. Silva, R. Neves, J. de Brito, R. Dhir, Carbonation behaviour of recycled
aggregate concrete, Cem. Concr. Compos. 62 (2015) 22–32.
[17] Y. Qin, H. Yang, Carbonation dominates the acid intake of recycled concrete
aggregate subjected to intermittent leaching, Constr. Build. Mater. 89 (2015)
110–114.
[18] J. Geng, J. Sun, Characteristics of the carbonation resistance of recycled fine
aggregate concrete, Constr. Build. Mater. 49 (2013) 814–820.
818 G. Pan et al. / Construction and Building Materials 154 (2017) 810–818
[19] D. Hermawan, T. Hata, K. Umemura, S. Kawai, W. Nagadomi, Y. Kuroki, Rapid
production of high-strength cement-bonded particleboard using gaseous or
supercritical carbon dioxide, J. Wood Sci. 47 (4) (2001) 294–300.
[20] L. Lange, C. Hills, A. Poole, The influence of mix parameters and binder choice
on the carbonation of cement solidified wastes, Waste Manage. 16 (8) (1996)
749–756.
[21] D. Johnson, C. MacLeod, P. Carey, C. Hills, Solidification of stainless steel slag by
accelerated carbonation, Environ. Technol. 24 (6) (2003) 671–678.
[22] M.F. Bertos, X. Li, S. Simons, C. Hills, P. Carey, Investigation of accelerated
carbonation for the stabilisation of MSW incinerator ashes and the
sequestration of CO2, Green Chem. 6 (8) (2004) 428–436.
[23] J. Sun, M.F. Bertos, S.J. Simons, Kinetic study of accelerated carbonation of
municipal solid waste incinerator air pollution control residues for
sequestration of flue gas CO2, Energy Environ. Sci. 1 (3) (2008) 370–377.
[24] S. Monkman, Y. Shao, Assessing the carbonation behavior of cementitious
materials, J. Mater. Civ. Eng. 18 (6) (2006) 768–776.
[25] S. Monkman, Y. Shao, Carbonation curing of slag-cement concrete for
binding CO2 and improving performance, J. Mater. Civ. Eng. 22 (4) (2009)
296–304.
[26] B. Zhan, C.S. Poon, Q. Liu, S. Kou, C. Shi, Experimental study on CO2 curing for
enhancement of recycled aggregate properties, Constr. Build. Mater. 67 (2014)
3–7.
[27] C. Wang, J. Xiao, G. Zhang, L. Li, Interfacial properties of modeled recycled
aggregate concrete modified by carbonation, Constr. Build. Mater. 105 (2016)
307–320.
[28] S.C. Kou, B.J. Zhan, C.S. Poon, Use of a CO2 curing step to improve the properties
of concrete prepared with recycled aggregates, Cem. Concr. Compos. 45 (2014)
22–28.
[29] J. Zhang, C. Shi, Y. Li, X. Pan, C.S. Poon, Z. Xie, Performance enhancement of
recycled concrete aggregates through carbonation, J. Mater. Civ. Eng. 27 (11)
(2015) 04015029.
[30] B.J. Zhan, C.S. Poon, C.J. Shi, Materials characteristics affecting CO2 curing of
concrete blocks containing recycled aggregates, Cem. Concr. Compos. 67
(2016) 50–59.
[31] G.T., Recycled fine aggregate for concrete and mortar [S], 2010.
[32] G.T., Sand for construction [S], 2011.
[33] G.T., Ready-mixed mortar [S], 2011.
[34] J.T., Standard for test method of basic properties of construction mortar [S],
2009.
[35] H. Cui, W. Tang, W. Liu, Z. Dong, F. Xing, Experimental study on effects of CO2
concentrations on concrete carbonation and diffusion mechanisms, Constr.
Build. Mater. 93 (2015) 522–527.
[36] A. Leemann, F. Moro, Carbonation of concrete: the role of CO2 concentration,
relative humidity and CO2 buffer capacity, Mater. Struct. 50 (1) (2016).
[37] D. Silva, V. John, J. Ribeiro, H. Roman, Pore size distribution of hydrated cement
pastes modified with polymers, Cem. Concr. Res. 31 (8) (2001) 1177–1184.
[38] H.M. Jennings, Design of high strength cement based materials: part 2
microstructure, Mater. Sci. Technol. 4 (4) (1988) 285–290.
[39] P.K. Mehta, Concrete. Structure, Properties and Materials, Prentice Hall Inc,
1986. pp. 367–378.