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Article history: Limestone powder improves concrete early-age strength while fly ash improves concrete late-age
Received 25 September 2017 strength due to its pozzolanic reaction. The optimal mixture of cement, fly ash, and limestone is crucial
Received in revised form 6 January 2018 for material design of ternary blended concrete. This research presents a simulation program for evalu-
Accepted 9 January 2018
ating the hydration and strength optimization of ternary blended concrete. The simulation program
begins with a kinetic hydration model which simulates the hydration of cement-fly ash-limestone tern-
ary blends. The hydration model considers the mutual effects among reactions of cement, fly ash, and
Keywords:
limestone by means of the contents of calcium hydroxide and capillary water. The individual reaction
Fly ash
Limestone
degrees of components of ternary blends are calculated from the hydration model. Furthermore, the com-
Hydration pressive strength growth of hydrating ternary blended concrete is calculated by means of gel-space ratio
Model and Powers’ strength theory. Finally, based on parameter studies, the optimal combinations of cement, fly
Strength optimization ash, and limestone at different ages are determined. The proposed numerical procedure is valuable for
making composite cements as it pertains to compressive strength and environment regulations.
Ó 2018 Elsevier Ltd. All rights reserved.
1. Introduction stone powder. Scholer et al. [3] found that a limestone content of
2–5% leads to the stabilization of monocarbonate and ettringite
Fly ash and limestone are more and more utilized in producing which can increase the volume of hydration products and increase
high performance concrete in the modern concrete industry. Fly the strength. Bentz et al. [4] found that nano-limestone can accel-
ash and limestone present different effects on strength develop- erate the early age hydration of cement and reduce the setting time
ment of concrete. Fly ash can enhance the long-term age strength of fly ash blended concrete. Thongsanitgarn et al. [5,6] found that
of concrete due to a pozzolanic reaction while limestone can cement-fly ash-limestone ternary blended concrete presents
enhance the young-age strength of concrete because limestone higher strength compared to cement-fly ash binary concrete. Lime-
can accelerate cement hydration. When limestone and fly ash are stone with finer particle size is effective to speed up cement-fly ash
used together, due to the synergy effect, the individual deficiencies hydration. Celik et al. [7,8] found that concrete containing high vol-
can be compensated [1]. ume fly ash and limestone has high workability, high late age
Abundant experimental and theoretical studies have been per- strength, high chloride resistance, and low global warming poten-
formed on cement-fly ash-limestone ternary blended concrete. tial. Ghrici et al. [9] found that natural pozzolana did not change
Weerdt et al. [2] found that the additional aluminum from the the sulfate resistance of limestone cement, natural pozzolana
fly ash pozzolanic reaction amplified the chemical reaction of lime- improved hydrochloric acid resistance, and limestone improved
sulfuric acid resistance.
https://doi.org/10.1016/j.conbuildmat.2018.01.058
0950-0618/Ó 2018 Elsevier Ltd. All rights reserved.
X.-Y. Wang / Construction and Building Materials 166 (2018) 130–140 131
Compared with abundant experimental studies of ternary temperature on rate of hydration of cement is recognized as fol-
blended concrete [2–9], theoretical studies of ternary blended con- lowing Arrhenius’s law [14–16]. For high strength concrete, degree
crete are relatively limited. Gao et al. [10] put forward an analytical of hydration is reduced due to the withdrawal of capillary water.
modeling about the hydration of cement-slag-limestone blends. The water withdrawal mechanism is considered through ðSw =S0 Þ
The local water to cement ratio and water transport in the interfa- and C wfree in Eq. (1). ðSw =S0 Þ describes the decrease in contact area
cial transition zone was simulated. Maekawa et al. [11] proposed a between cement particle and ambient capillary water, and C wfree
computational platform which can assess the time-dependent describes the decrease in capillary water concentration.
mechanics and durability mechanics of concrete structures. The Similarly with hydration of cement, fly ash reaction also con-
couplings among hydration, mass transport, and damage evolution sists of three stages [14–16], initial dormant stage, chemical-
were considered. However, Gao et al. [10] and Maekawa et al.’s reaction related stage, and diffusion related stage. In addition, fly
[11] studies do not consider the chemical reaction of limestone ash reaction is dependent on calcium hydroxide content in
in ternary blended concrete. Bentz [12] proposed a model which cement-fly ash binary blends. The equation of fly ash reaction is
simulated the dilution, nucleation, and chemical effects of lime- simplified written as below [14–16]:
stone additions in cement-limestone binary blends. Weerdt et al.
daFA mCH ðtÞ
[13] made a thermodynamic modeling of hydration of cement-fly ¼ f ðkdFA ðTÞ; DeFA ðTÞ; krFA ðTÞ; r FA0 Þ ð2Þ
ash-limestone ternary blends. The volumetric phase fractions of dt P
the hydrating paste were calculated using Gibbs Energy Minimiza- where dadtFA is fly ash reaction rate, kdFA is rate of coefficient in initial
tion Software (GEMS) program. However, the thermodynamic dormant stage of fly ash, DeFA is rate of coefficient in diffusion
modeling in the Weerdt et al. study [13] mainly focuses on the
related stage of fly ash, krFA is rate of coefficient in reaction related
chemical aspects of ternary blended concrete. Regarding the opti-
stage of fly ash, r FA0 is unreacted fly ash particles radius, mCH ðtÞ is
mal combinations of cement, fly ash, and limestone in ternary
the content of calcium hydroxide, P is fly ash content in proportions
blended concrete, current models [10–13] still do not cover this
of concrete mix.
point.
The time-dependent cement or fly ash reaction degrees can be
To avoid the flaws of current studies, this research presents a
calculated using the cement-fly ash binary hydration model. In
hydration based simulation program to assess the strength growth
addition, the thermal properties, mechanical properties, and dura-
and optimal combinations of ternary blended concrete. The
bility of fly ash blended concrete can be evaluated using reaction
strength is evaluated considering the influences from reactions of
degree of individual component of binders. The cement-fly ash bin-
cement, fly ash, and limestone. The optimal combinations are
ary hydration model is multiply validated using experimental data
determined based on parameter studies of the hydration-
for concrete with various proportions of mix and curing conditions.
strength integrated model.
However, because the cement-fly ash binary hydration model does
not consider the effect of limestone, binary hydration model can-
2. Simulation of the hydration of cement-fly ash-limestone not analyze the hydration of cement-fly ash-limestone ternary
ternary blends concrete.
2.1. Simulation of the hydration of cement-fly ash binary blends 2.2. Limestone powder reaction mode
Our previous studies [14–16] presented a kinetic hydration Bentz [12] reported that the addition of limestone presents
model for concrete containing fly ash. This kinetic hydration model dilution, nucleation, and chemical effects on cement hydration.
includes three sub-models, i.e. model for hydration of cement, The dilution effect happens when limestone substitutes partial
model for reaction of fly ash, and model for mutual effects between cement, cement content decreases and water to cement ratio
reactions of cement and fly ash. The cement hydration model con- increases correspondingly. The nucleation effect is the fact that
siders the kinetic stages involved in the hydration of cement, such limestone may work as a nucleation site of hydrating
as initial dormant stage, chemical-reaction related stage, and diffu- cement. Hydration of cement can accelerate due to the nucle-
sion related stage. The cement hydration model also considers the ation effect. The chemical effect is the formation of monocar-
water withdrawal on account of the lack of capillary water regard- boaluminate due to the limestone reaction in preference to a
ing high strength concrete. The equation of cement hydration is monosulfoaluminate.
simplified and written as follows [14–16]: In this research, the dilution effect of limestone powder can be
C0
considered by W term in C wfree of Eq. (1). Regarding the nucleation
da 0
¼ f ðkd ðTÞ; De ðTÞ; kr ðTÞ; r0 Þ C wfree ðSw =S0 Þ ð1Þ effect, Maekawa et al. [11] and Wang [16] proposed that the nucle-
dt
ation effect of limestone relates to the ratio of surface area of
where ddta is rate of hydration, kd is rate of coefficient in initial dor- cement particles to that of limestone powder. The nucleation effect
mant stage, T is curing temperature, kr is rate of coefficient in reac- indicator of limestone powder can be written as follows [16]:
tion related stage, De is rate of coefficient in diffusion related stage,
LS0 SLS
r 0 is unreacted cement particles radius, Sw means the effective con- Lr ¼ ð3Þ
C 0 SC
tact area between the surrounding capillary water and cement par-
ticles [14–16], S0 means the total area if cement hydration products where Lr denotes the indicator of the nucleation effect from lime-
progress unconstrained, C wfree is capillary water content stone addition, LS0 denotes the limestone mass in proportions of
r
(C wfree ¼ W 0 0:4C 0a
where C 0 is cement content in concrete mix- concrete mix, SLS denotes the specific surface (Blaine) of limestone,
W0
and SC denotes the specific surface (Blaine) of cement. Maekawa
ing proportions, W 0 is the content of water in the proportions of et al. [11] reported that the nucleation effect of limestone is signif-
concrete mix, r (r ¼ 2:6 4 W
C0
0
) is an empirical factor considering icant in the reaction related stage and the diffusion related stage. In
the approachability of capillary water from outer hard shell to inner our former study [16], based on the experimental data of hydration
anhydrous part of cement particles). degree of cement in cement-limestone binary blends, Wang [16]
The rate coefficients kd , kr , and De can be determined based on proposed that the nucleation effect of limestone powder can
compound compositions of cement [14–16]. The effect of described as follows:
132 X.-Y. Wang / Construction and Building Materials 166 (2018) 130–140
krLS ¼ kr ð1 þ 1:2Lr Þ ð4Þ to binder ratio, and curing temperature, will affect the limestone
reaction [19,20]. Considering these points, we propose a more
DeLS ¼ De ð1 þ 1:2Lr Þ ð5Þ general equation for determining the reaction degree of limestone
as follows:
where krLS is the updated phase boundary reaction coefficient in
cement-limestone blends, 1.2 is enhance coefficients of kr [16], aLS ¼ aLS1 m1 m2 m3 m4 m5 m6 ð7Þ
DeLS is the updated diffusion coefficient in cement-limestone blends,
and 1:2 is enhance coefficients of De [16]. where m1 considers the effect of limestone replacement ratios on
Ipavec et al. [17] measured the formation of carboaluminate reaction degree of limestone, m2 considers the effect of limestone
phases in limestone powder blended paste (the water to binder fineness, m3 considers the effect of cement fineness, m4 considers
ratio is 0.5, the limestone replacement ratio is 0.2, and curing tem- the effect of fly ash addition, m5 considers the effect of water to bin-
perature is 20 °C). The contents of carboaluminate phases were der ratio, and m6 considers the effect of curing temperature. For the
measured at 1, 3, 7, 15, 28, and 100 days. Monocarboaluminate is case of Ipavec et al.’s [17] study, all of these influencing factors
the main hydration product of limestone at late ages. Based on equal to 1.
monocarboaluminate contents, we suggest that the limestone
reaction degree can be calculated as below: 2.2.1. Effect of limestone replacement ratios
Antoni et al. [20] reported that as limestone replacement ratio
aLS1 ¼ 0:0087 lnðtÞ 0:0265 ðt > 21Þ ð6Þ increases, the reaction degree of limestone powder decreases.
where aLS1 is the reaction degree of limestone powder, and t is age Based on Antoni’s [20] results, we found that the reaction degree
(hours). The evaluation results about reaction degree of limestone of limestone is approximately an inverse proportional function of
are shown in Fig. 1. Fig. 1 shows that the reaction degree of limestone replacement ratio. Hence, we assume that m1 ¼ 0:2 LS0 .
C 0 þLS0
limestone is a logarithm function of time, which is similar to the
relation between hydration degree of cement and curing age
2.2.2. Fineness of limestone
[14–16]. Fig. 1 also shows that the reaction of limestone starts after
Aqel and Panesar [19] reported that when average particle size
about 21 h, not immediately after mixing. Bentz [12] proposed that
of limestone powder decreases, the reactivity of limestone
the limestone chemical reaction can be written as 3ðCaOÞ3 ðAl2 O3 Þ
increases. Based on Aqel’s study [19] about the relation between
CaSO4 12H2 O þ 2CaCO3 þ 18H2 O ! 2ðCaOÞ3 ðAl2 O3 Þ CaCO3 11H2 O þ
reaction degree and particle size of limestone, we assumed that
ðCaOÞ3 ðAl2 O3 Þ 3CaSO4 32H2 O. Bentz’s [12] study shows that the
m2 ¼ 1:0131 0:0144 dLS where dLS is average diameter of
limestone reaction starts only when the initial calcium sulfate
limestone.
is fully consumed and the formed ettringite phase begins to convert
to the AFm phase. Lothenbach [18] reported that after about 1 day,
the reaction of limestone starts. The starting time of limestone in 2.2.3. Fineness of cement
Lothenbach’s [18] study (1 day) is similar to our study (21 h). In Aqel and Panesar [19] found that when the Blaine surface of
addition, by using Eq. (6), we find that at the age of 180 days, the cement increases, the average reaction degree of limestone also
reaction degree of limestone is about 4.6%, which is similar to increases. Based on Aqel’s [19] study, we assumed that that
the results of Bentz’s study [12] (Bentz [12] proposed that for m3 ¼ 0:55 SSC1C þ 0:45 where SC1 is the Blaine surface of cement used
concrete with 20% limestone, at the age of 180 days, about 5% in Ipavec et al.’s [17] study.
limestone reacted). The reactivity of limestone is much lower
compared to cement or fly ash [14–16]. 2.2.4. Fly ash additions
On the other hand, we should notice that Eq. (12) is only valid Weerdt et al. [2] reported that due to the high aluminum con-
for Ipavec et al.’s [17] study (water to binder ratio was 0.5, lime- tent in fly ash, the limestone reaction in cement-fly ash-
stone replacement ratio was 0.2, and curing temperature was limestone ternary blends is enhanced. We proposed that the influ-
_20 °C). Limestone reaction is a complex process and relates to ence of fly ash on limestone addition can be described as
abundant factors. The factors, such as limestone replacement
m4 ¼ 1 þ AlAlFAC aaCFA0P, where AlFA and AlC are aluminum contents in fly
ratios, fly ash addition, limestone fineness, cement fineness, water
ash and cement respectively. AlFA aFA P and AlC aC 0 are reacted alu-
minum contents from fly ash reaction and cement reaction
respectively.
Table 3
Properties of binders.
SiO2 Al2O3 Fe2O3 CaO MgO SO3 K2O Na2O Blaine surface
(%) (%) (%) (%) (%) (%) (%) (%) (m2/kg)
Cement 20.0 5.4 3.1 60.6 2.9 1.5 1.2 0.5 450
Fly ash 50.0 23.9 6.0 6.3 2.1 0.4 1.4 0.6 450
Limestone 12.9 2.7 2.0 42.3 1.8 – 0.6 0.5 810
X.-Y. Wang / Construction and Building Materials 166 (2018) 130–140 135
100 50
control FA35%-cal
reaction degree of cement %
40 20
20 10
0 -2 0 2 4
0 0 2 4
10 10 10 10 10 10 10
curing age(hours) curing age(hours)
0.05
0
0 1000 2000 3000 4000 5000
curing age(hours)
0.4
0.2
0 0 2
10 10
time(hours)
+ 35% fly ash), due to the dilution effect from fly ash addition, blends. The sequence of reaction degree of cement from high to
cement reaction degree is higher than control paste. The ternary low is ternary blends, fly ash binary blends, limestone binary
blends (65% cement + 30% fly ash + 5% limestone) has a higher blends, and control specimen. The proposed hydration model can
reaction degree of cement than the control specimen or binary reproduce this sequence of reaction degree of cement.
136 X.-Y. Wang / Construction and Building Materials 166 (2018) 130–140
Fig. 3b shows fly ash reaction degree in binary or ternary lower compared to binary mix (5% limestone + 95% cement). This is
blended concrete. When 5% limestone is added, the fly ash reaction because the cement to limestone ratio is lower in ternary mix
degrees in binary blends (65% cement + 35% fly ash) or ternary compared to binary mix (related to influencing factor m1 of
blends (65% cement + 30% fly ash + 5% limestone) are similar. First, limestone reaction).
the limestone addition can lower CH content which will decrease Based on reaction degree of binders and volumetric ratio
the rate of fly ash reaction. Second, when partial fly ash is replaced between reaction products and binders, the volumetric phase frac-
by limestone, the ratio between cement and fly ash increases tions of hydrating ternary paste can be calculated. Fig. 3f shows the
which will increase the rate of fly ash reaction. On account of the volumetric phase fractions of ternary paste (cement 65% + fly ash
simultaneous effects of increasing factor and decreasing factor, 20% + limestone 15%). Because cement hydrates much quicker
fly ash reaction degrees in binary blends or ternary blends are compared to fly ash, less cement is remained compared to fly
similar. ash. On account of the depositing of reaction products, capillary
Fig. 3c shows CH content in limestone binary blends (95% porosity decreases as hydration evolves.
cement + 5% limestone) and control concrete. On account of the
consumption of CH from limestone addition, limestone binary 3.2. Strength development and strength optimization of concrete
blends present lower CH contents compared to control
specimen. Fig. 3d shows that regarding cement-limestone binary Based on the reaction degree of binders, the gel-space ratio of
blends, the reaction degree of limestone decreases as limestone hardening concrete can be determined. Moreover, concrete com-
content increases. Fig. 3e shows that at late age, fly ash (5% pressive strength can be calculated using Powers’ strength theory.
limestone + 30% fly ash + 65% cement) can increase the reaction By using experimental data of concrete compressive strength with
degree of limestone compare to limestone-cement binary blends various mixing proportions at different ages, these coefficients a1,
(5% limestone + 95% cement). This is because of the high aluminum a2, a3, b1, b2, and b3 can be calibrated. The values of intrinsic
content in fly ash (related to influencing factor m4 of limestone strength of cement, fly ash, and limestone are 184.89 MPa,
reaction). While at early-age, limestone powder reaction degree 207.11 MPa, and 122.09 MPa respectively. The values of strength
in ternary mix (5% limestone + 30% fly ash + 65% cement) is slightly exponent of cement, fly ash, and limestone are 2.45, 3.04, and
0.8
OPC
10%ls 1
0.6 20%ls
30%ls OPC
10%ls
0.4 20%ls
0.5 30%ls
0.2
0 0
0 50 100 150 200 0 50 100 150 200
curing age(days) curing age(days)
60
compressive strength(MPa)
10%LS
15%LS
50
20%LS 1
25%LS
40
30%LS
35%LS
30
exper. res.
0.5 OPC
20
10%ls
20%ls
10
30%ls
0 -1 0 1 2
0 -1 0 1 2
10 10 10 10 10 10 10 10
curing age(days) curing age(days)
2.39 respectively. These coefficients do not change for various mix- from that of relative compressive strength (Fig. 4d). The compres-
ing proportions of concrete (total 21 mixtures) and various curing sive strength relates to not only degree of hydration, but also the
ages (from early age (1 day) to late ages (28, 90, and 140 days)). A contents of cement and limestone.
total of 84 experimental data about compressive strength (21 * 4 = The analysis of strength development of cement-fly ash binary
84) are used in this research. blends is shown in Fig. 5. Fig. 5a shows fly ash reaction degree in
The development of strength of cement-limestone binary binary blends. As fly ash content increases, the alkali activation
blends is shown in Fig. 4. Fig. 4a shows cement reaction degree effect becomes weaker, and fly ash reaction degree decreases.
in cement-limestone binary blends. As limestone content Fig. 5b shows that the analysis results generally conform to exper-
increases, due to dilution effect and nucleation effect, cement imental data. Fig. 5c shows that at early-age, fly ash additions
hydration degree increases. In this study, the relative hydration lower concrete strength. This is because fly ash reaction rate is
degree of cement means the ratio of hydration degree of cement much lower compared to cement (shown in Fig. 3b and a). While
in binary blends to that in plain specimen, and the relative strength at late age, due to the progress of the fly ash reaction, the strength
means the ratio of compressive strength of binary blends to that of of concrete containing fly ash can surpass the strength of plain con-
plain specimen. As shown in Fig. 4b, as limestone content crete. As fly ash content increases, fly ash reaction degree becomes
increases, relative reaction degree of cement also increases. lower (shown in Fig. 5a), and age akin to exceed strength is going
Fig. 4c shows that the analysis results about compressive strength to be delayed.
generally conform to experimental data. Fig. 4d shows that at Fig. 6 presents the analyzed compressive strength of ternary
early-age, limestone addition can increase concrete strength. This blends. At long term age, the specimens containing higher fly ash
is because of the acceleration of hydration of cement. While at late content (Fig. 6a and b) have higher compressive strength than
age, due to dilution effect, limestone blended concrete presents those containing lower fly ash contents (Fig. 6e and f). The results
lower strength compared to control concrete. It should be noted of analysis and tests are shown in Fig. 7. The relative coefficient
that the trend of relative degree of hydration (Fig. 4b) is different between analysis and experiment results is 0.99, and the root
fly ash binary blended concrete fly ash binary blended concrete
1 70 control
10%Fa
5%FA
20%Fa 60
compressive strength(MPa)
10%FA
reaction degree of fly ash
0.8 35%Fa
15%FA
50
20%FA
0.6 25%FA
40
30%FA
30 35%FA
0.4 exper. res.
20
0.2
10
0 -1 0 1 2
0 -1 0 1 2
10 10 10 10 10 10 10 10
curing age(days) curing age(days)
OPC
10%Fa
0.5 20%Fa
35%Fa
0 -1 0 1 2
10 10 10 10
curing age(days)
mean square error (RMSE) between analysis and experiment is Based on the hydration-strength integrated model, we perform
1.48 MPa. The analysis results generally conform to the experi- parameter studies about strength of ternary blended concrete with
mental data. The proposed simulation program can evaluate the various binder combinations at various ages. As shown in Fig. 8a
strength of binary and ternary concrete at both early ages and late (0.3 day) and Fig. 8b (0.5 day), because limestone addition can
ages. improve concrete early age strength, concrete with higher
compressive strength(MPa)
50 50
40 40
30 30
20 20
10 10
0 -1 0 1 2
0 -1 0 1 2
10 10 10 10 10 10 10 10
curing age(days) curing age(days)
compressive strength(MPa)
50 50
40 40
30 30
20 20
10 10
0 -1 0 1 2
0 -1 0 1 2
10 10 10 10 10 10 10 10
curing age(days) curing age(days)
compressive strength(MPa)
50 50
40 40
30 30
20 20
10 10
0 -1 0 1 2
0 -1 0 1 2
10 10 10 10 10 10 10 10
curing age(days) curing age(days)
70 12
50
8
40
6
30 0.5 day
4 28 days 90 days
20
10 2
0 0
0 10 20 30 40 50 60 70 0 5 10 15 20 25
experimental results(MPa) optimum fly ash replacement ratio %
Fig. 7. Comparison between analysis and experimental results. Fig. 9. Optimum combinations of ternary blends.
limestone content and lower fly ash contents has the highest the highest strength of all mixes. As shown in Fig. 9, from early-
strength of all other mixes. As shown in Fig. 8d (90 days), because age to late age, the optimal combination for ternary blends shifts
fly ash can improve concrete late age strength, concrete with from high limestone-low fly ash zone to high fly ash-low limestone
higher fly ash contents and lower limestone contents presents zone.
11
25 25 15
fly ash replacement ratio %
10 14
20 20
13
9
15 15
12
8
10 10 11
7 10
5 5
9
6
0 0
0 2 4 6 8 10 12 0 2 4 6 8 10 12
limestone replacement ratio % limestone replacement ratio %
(a) 0.3 day. (b)0.5 day.
25 48 25 57
fly ash replacement ratio %
56
20 46 20
55
44 54
15 15
53
10 42 10 52
51
5 40 5
50
0 38 0 49
0 2 4 6 8 10 12 0 2 4 6 8 10 12
limestone replacement ratio % limestone replacement ratio %
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