buildings
Article
Volume Stability of Cement Paste Containing Limestone Fines
Jamal Khatib * , Rawan Ramadan, Hassan Ghanem






Citation: Khatib, J.; Ramadan, R.;
Ghanem, H.; Elkordi, A. Volume
Stability of Cement Paste Containing
Limestone Fines. Buildings 2021, 11,
366. https://doi.org/10.3390/
buildings11080366
Academic Editor: Marco Di Ludovico
Received: 28 July 2021
Accepted: 17 August 2021
Published: 19 August 2021
Publisher’s Note: MDPI stays neutral
with regard to jurisdictional claims in
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iations.
Copyright: © 2021 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Buildings 2021, 11, 366. https://doi.org/10.3390/buildings11080366
and Adel Elkordi
Faculty of Engineering, Beirut Arab University, Beirut P.O. Box 11-5020, Lebanon;
rawanramadan178@gmail.com (R.R.); h.ghanem@bau.edu.lb (H.G.); a.elkordi@bau.edu.lb (A.E.)
* Correspondence: j.khatib@bau.edu.lb
Abstract: The common cause of cracking in cement paste is shrinkage due to different reasons, such as
loss of water and chemical reactions. Incorporating limestone fines (LF) as a cement replacement can
affect the shrinkage of the paste. To examine this effect, five paste mixes were prepared with 0, 5, 10,
15 and 20% LF as a cement replacement and with a water-to-binder ratio (w/b) of 0.45. Four volume
stability tests were conducted for each paste: chemical, autogenous and drying shrinkage and
expansion. Chemical shrinkage was tested each hour for the first 24 h and thereafter every 2 days
for a total period of 90 days. The drying shrinkage, autogenous shrinkage and expansion were
monitored every 2 days until 90 days. The results showed that replacing 15% LF enhanced the
chemical shrinkage of the paste. However, autogenous shrinkage of the paste was found to increase
between 0 and 10% LF and decline sharply at 15 and 20% LF. Drying shrinkage was found to increase
with the increase in LF content. Expansion exhibited little variation between 0 and 10% LF and an
increase for replacement above 15% LF. These results are discussed in terms of the formation of
hydration products and self-desiccation due to hydration.
Keywords: limestone fines; chemical shrinkage; autogenous shrinkage; drying shrinkage; expansion
1. Introduction
Concrete’s tendency to crack is historically recognized as inevitable. Therefore, most
current concrete buildings tend to be affected by the formation of cracks. In order to reduce
cracking and improve building materials, the concrete shrinkage during construction needs
to be controlled, as this will have an impact on the concrete’s durability. There are different
types of shrinkage responsible for these cracks such as chemical, autogenous and drying
shrinkage. Drying shrinkage is defined as the contracting of a hardened concrete caused
by the removal of free water from the concrete, which is caused by the changes in relative
humidity and temperature [1]. This can be controlled by using concrete with a lower
w/c ratio or by adding supplementary cementitious materials (SCMs) that lead to its
reduction [2]. Chemical shrinkage is well-defined as the internal volume change of cement
paste resulting from the hydration of cementitious materials [3]. This is affected by the
temperature and cement composition. Traditionally, chemical shrinkage was tested by
three main measurement methods such as dilatometry, pycnometry and gravimetry. Many
authors prefer using the dilatometry method to monitor chemical shrinkage [4–14]. The
dilatometry method is based on measuring a drop of water in a hydrating cement paste
through a graduated pipette [15]. Autogenous shrinkage is the macroscopic reduction in
the external dimensions of cement particles during curing without any loss of moisture that
occurs simultaneously with chemical shrinkage [16]. The cement content and temperature
are the major factors affecting this type of shrinkage. These are controlled by the change
in internal curing of the system due to self-dehydration at lower water-to-cement ratios
(w/c < 0.4) [17]. Expansion of concrete occurs if exposed to water or an excessive amount
of moisture. The hydration process is liable for water withdrawal from the capillary pores
that are present within the concrete. Through the first hours of hydration, the capillary
activities can be considered negligible. Therefore, the autogenous shrinkage is mainly
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Buildings 2021, 11, 366 2 of 17

corresponding to the chemical shrinkage [18]. The phenomenon of water withdrawal from
the capillary pores to bring out the hydration is called “self-desiccation”. When specimens
are cured in water, they show continuous expansion with time, even though the total
system volume continues to decline [9,19].
Limestone is a hard sedimentary rock with multiple uses consisting of calcium carbon-
ate (CaCO3 ). It is mostly crushed and used as a construction material. Some contractors
throughout a wide range of industries are interested in gathering up crushed limestone
to complete their projects. Its main applications are in concrete, road base, railroad bal-
last, driveways and pipe bedding because of its strength, practicality and durability [20].
Many authors examined the effect of LF as a cement or aggregate replacement on concrete
shrinkage. It was found that incorporating LF as a cement replacement affected the drying
shrinkage of the concrete [21–24]. Aquino et al. [25] proved that integrating LF as a fines
aggregate replacement could decrease the drying shrinkage in concrete. Another study
conducted by Valcuende et al. [26] showed that the drying shrinkage increased as the LF
content increased. Chemical shrinkage is also considered a point of controversy among
researchers. The presence of limestone filler produced an acceleration of chemical shrink-
age and the hydration process in the early ages. This filler acts as the nucleation sites for
hydrates [27]. In addition to that, combining 5% LF increased the chemical shrinkage [28].
On the other side, Wang et al. [29] proved that incorporating LF reduced the chemical
shrinkage. The inclusion of LF will definitely reduce the cement content and lead to a rise
in the W/C ratio. Therefore, the internal humidity of concrete increases, which results in
reducing the concrete shrinkage. Adding a small content of LF as a cement replacement
improves the degree of hydration and reinforces the hydration of concrete. Hence, adding
LF enhances the autogenous shrinkage [30]. However, Bentz et al. [31] proved that adding
10% LF with a particle size of 16 µm as a cement replacement diminished the autogenous
shrinkage of the concrete.
According to the premises mentioned above, there is a substantial amount of research
on chemical, autogenous and drying shrinkage and expansion of concrete and paste con-
taining SCM [32–43] and some on chemical shrinkage [44,45]. However, there is hardly any
research to compare the chemical shrinkage of paste with other types of shrinkage such as
autogenous shrinkage, drying shrinkage and expansion. In addition, cement manufactur-
ing contributes about 7% of global CO2 emissions [23]. Therefore, partial replacement of
cement with LF will reduce such emissions and contribute toward sustainable development.
Therefore, the aim of this paper is to examine the volume stability of pastes containing LF.
Volume stability includes chemical, autogenous and drying shrinkage as well as expansion.

2. Materials and Methods

2.1. Materials
Portland cement PA-L 42.5 N type I was used in this study. This type of cement
contained 0.5% free limestone. The incorporated raw limestone was extracted from Lebanon
quarries. This limestone was first ground and then sieved until reaching a fines particle size
below 300 µm. The particle size distributions of the limestone and cement are illustrated in
Figure 1. The limestone density was 2.7 g/cm3 . The chemical properties for the cement
and limestone are shown in Table 1. The physical properties of the cement are presented
in Table 2.
 Initial Setting Time (min) 232
Final Setting Time (min) 282
Soundness (mm) 0
Blaine (cm2/g) 3998
Buildings 2021, 11, 366 3 of 17
Water Demand 26.6

100%

80%

Cumulative % passing
60%

40%

20%

0%
0.01 0.1 1 10 100
Diameter (mm)
Figure 1. Particle size distribution of the LF and cement.
Figure 1. Particle size distribution of the LF and cement.
Table 1. Chemical composition of cement and LF.
2.2. Mix Proportions
Oxidethis experiment,
During SiO2 AL 2 Owith
LF 3 Fe52 O CaO
replacement
3 MgO of cement
levels SO3 Na5,
(0, 2 O10, 15
K2and
O 20%)
L.O.I
were incorporated
Cement % in paste specimens
18.53 3.93 with a61.78
3.06 w/b ratio1.74
of 0.45.2.92
Five paste
0.18mixes were em-
0.47 6.3
LF % 5.17 1.65 0.77 50.98 0 0.21 0.18 0.12
ployed. The total number of specimens tested was 40, with 10 specimens for each type of 39.64
shrinkage (chemical, autogenous and drying shrinkage and expansion). The details of the
paste mix ratio are presented in Table 3.
Table 2. Physical properties of the cement.

Table 3. Paste mix proportions.

Initial Setting Time (min) 232
Final
Paste Setting Time (min) Cement
Code LF 1 282 W/B Ratio
P0%Soundness (mm) 1 0 0 0.45
P5% 0.95 0.05 0.45
Blaine (cm2 /g) 3998
P10% 0.9 0.1 0.45
P15% Water Demand 0.85 0.15 26.6 0.45
P20% 0.8 0.2 0.45
1 Limestone fines.
2.2. Mix Proportions
During this experiment, LF with 5 replacement levels of cement (0, 5, 10, 15 and 20%)
2.3. Specimen Preparation and Test Procedure
were incorporated in paste specimens with a w/b ratio of 0.45. Five paste mixes were
2.3.1. ChemicalThe
employed. Shrinkage
total number of specimens tested was 40, with 10 specimens for each type
ofAshrinkage
chemical (chemical, autogenous
shrinkage test and drying
was performed shrinkage
according and expansion).
to ASTM C 1608 [46]. The details
chem- of
the paste mix ratio are presented in Table 3.
ical shrinkage specimens and test set-up are shown in Figure 2a,b, respectively. The ce-
ment and LF were dry mixed for 2 min and then poured with water. After that, 30 gm of
Table
paste Paste mix
was3. placed in aproportions.
250-mL glass bottle for each mix, which corresponded to a depth of
Paste Code Cement LF 1 W/B Ratio
P0% 1 0 0.45
P5% 0.95 0.05 0.45
P10% 0.9 0.1 0.45
P15% 0.85 0.15 0.45
P20% 0.8 0.2 0.45
1 Limestone fines.
 Buildings 2021, 11, 366 4 of 17

Buildings 2021, 11, x FOR PEER REVIEW 4 of 18

2.3. Specimen Preparation and Test Procedure
2.3.1. Chemical Shrinkage
around 1.8Acm. chemical shrinkage
Subsequently, test graduated
a 2-mL was performed
pipetteaccording to ASTM
was inserted through C a1608
hole [46].
in a The
rubber stopper and filled with water. This level of water was considered the chemical The
chemical shrinkage specimens and test set-up are shown in Figure 2a,b, respectively.
cement
shrinkage andvalue
initial LF were
(i.e., dry mixed
zero). forend,
At the 2 min andof
a drop then poured
oil was addedwith
to water.
preventAfter that, 30 gm
any water
of pasteTwo
evaporation. wasreplicate
placed inspecimens
a 250-mL were
glass tested
bottle for
for each
each mix,
mix. which corresponded
One bottle filled withto a depth
wa-
of around 1.8 cm. Subsequently, a 2-mL graduated pipette was inserted
ter only playing the role of a control specimen was used to monitor any drop in the water through a hole in
a rubber stopper and filled with water. This level of water was considered
level due to several environmental conditions (e.g., temperature variation, stopper relax- the chemical
shrinkage initial value (i.e., zero). At the end, a drop of oil was added to prevent any water
ation or water absorption by the stopper or the bottle). The average value of the two read-
evaporation. Two replicate specimens were tested for each mix. One bottle filled with water
ings represented the chemical shrinkage. During the first 24 h, the drop of water was mon-
only playing the role of a control specimen was used to monitor any drop in the water level
itored every 1 h and then once every 2 days until a total period of 90 days. The volume
due to several environmental conditions (e.g., temperature variation, stopper relaxation
change (chemical shrinkage) was transformed to length change using the following equa-
or water absorption by the stopper or the bottle). The average value of the two readings
tion [19]:
represented the chemical shrinkage. During the first 24 h, the drop of water was monitored
every 1 h and then once every 2 days ∆V/Vuntil a total period of 90 days. The volume(1)
= 3 ∆L/L change
(chemical shrinkage) was transformed to length change using the following equation [19]:
The results obtained were expressed in micrometers/meter in order to be compared
with autogenous and drying shrinkage and expansion.
∆V/V = 3 ∆L/L (1)

(a) (b)
FigureFigure
2. (a) Chemical shrinkage
2. (a) Chemical specimens.
shrinkage (b) Chemical
specimens. shrinkage
(b) Chemical test set-up.
shrinkage test set-up.

The results
2.3.2. Autogenous obtained were expressed in micrometers/meter in order to be compared
Shrinkage
with autogenous
Autogenous shrinkage and drying shrinkage
specimens and expansion.
were prepared using a Hobart mixer and tested ac-
cording to ASTM
2.3.2. C192 [47].
Autogenous The specimens were cast in steel molds with dimensions of 25
Shrinkage
mm × 25 mm × 300 mm and kept for 24 h. After demolding, two demec points at 200 mm
Autogenous shrinkage specimens were prepared using a Hobart mixer and tested
on two sides of the specimens were applied. The length change was recorded using a dial
according to ASTM C192 [47]. The specimens were cast in steel molds with dimensions
gauge of
(Figure
25 mm3).×
The
25 specimens
mm × 300were thenkept
mm and placed
forin
24plastic bags
h. After (Figure 4).two
demolding, Thedemec
lengthspoints
of at
the specimens were recorded every 2 days for a total period of 90 days. The length changes
reported were the average values of four readings from two specimens for each mix.
Buildings 2021, 11, 366 5 of 17

200 mm on two sides of the specimens were applied. The length change was recorded
using a dial gauge (Figure 3). The specimens were then placed in plastic bags (Figure 4).
The lengths of the specimens were recorded every 2 days for a total period of 90 days. The
Buildings 2021, 11, x FOR PEER REVIEW
length changes reported were the average values of four readings from two specimens55 of
Buildings 2021, 11, x FOR PEER REVIEW
18
for
of 18
each mix.

Figure3.3.Dial
Dial gauge.
Figure 3. Dialgauge.
Figure gauge.

Figure 4. Autogenous and drying shrinkage specimens.

Figure4.4.Autogenous
Figure Autogenousand
anddrying
dryingshrinkage
shrinkagespecimens.
specimens.
2.3.3.Drying
2.3.3. Drying Shrinkage
2.3.3. DryingShrinkage
Shrinkage
The
The drying shrinkagewas
was testedaccording
according to ASTMC157 C157 [48].The
The specimenswere
were
Thedrying
dryingshrinkage
shrinkage wastested
tested accordingtotoASTMASTM C157[48]. [48]. Thespecimens
specimens were
cast in 25 mm × 25 mm × 300 mm steel molds. After 24 h, the specimens were placed in air
cast
castinin25
25mmmm× × 25 mm ××300
25 mm 300mmmmsteel
steelmolds.
molds.After
After2424h,h, the
the specimens
specimens were
were placed
placed ininair
at
air an average temperature of 25 °C◦ as shown in Figure 4. The procedure for taking the
at at
anan averagetemperature
average temperatureofof25
25°CCas asshown
shown inin Figure
Figure 4. 4. The
The procedure
procedureforfortaking
takingthe
the
readingsand
readings and frequencywaswas similartotothat
that forthe
the autogenousshrinkage
shrinkage specimens.
readings andfrequency
frequency wassimilar
similar to thatfor
for theautogenous
autogenous shrinkagespecimens.
specimens.
2.3.4.Expansion
2.3.4. Expansion
2.3.4. Expansion
Thepaste
The paste specimens
specimens were castcast in
in25 mm× ×
25mm 25 25
mm mm × 300
× 300 mm mm steelsteel
molds. Two speci-
molds. Two
The paste specimens were cast in 25 mm × 25 mm × 300 mm steel molds. Two speci-
specimens
mens for each
for each mix were
mix were prepared
prepared to measure
to measure expansion.
expansion. AfterAfter
24 h,24theh,specimens
the specimens
were
mens for each mix were prepared to measure expansion. After 24 h, the specimens were
were immersed
immersed in water
in water at a constant
at a constant temperature
temperature (20 ± (20
1 °C) 1 ◦shown
± as C) as shown in Figure
in Figure 5. The5.proce-
The
immersed for
procedure in water
takingatthe
a constant
readings temperature
and (20 ±was
frequency 1 °C) as shown
similar to in for
that Figure
the 5. The proce-
autogenous
dure for taking the readings and frequency was similar to that for the autogenous shrink-
dure for taking
shrinkage the readings and frequency was similar to that for the autogenous shrink-
specimens.
age specimens.
age specimens.
Buildings 2021, 11, 366 6 of 17
Buildings 2021, 11, x FOR PEER REVIEW 6 of 18

Figure5.5.Expansion
Figure Expansionspecimens.
specimens.

3.
3. Results
Results and
and Discussion
Discussion
3.1. Chemical Shrinkage
3.1. Chemical Shrinkage
The results for the chemical shrinkage (µm/m) over 90 days are presented in Figure 6.
The results for the chemical shrinkage (µ m/m) over 90 days are presented in Figure
For the purpose of comparison, the units of chemical shrinkage were converted to the
6. For the purpose of comparison, the units of chemical shrinkage were converted to the
same units as those for drying shrinkage, autogenous shrinkage and expansion (microme-
same units as those for drying shrinkage, autogenous shrinkage and expansion (microm-
ter/meter) using Equation (1). It should be noted that there is a 1-day difference between
eter/meter) using Equation (1). It should be noted that there is a 1-day difference between
chemical shrinkage and other shrinkages. Hence, the zero time for chemical shrinkage is
chemical shrinkage and other shrinkages. Hence, the zero time for chemical shrinkage is
the time immediately after placing, while the zero time for other shrinkage bars is the time
the time immediately after placing, while the zero time for other shrinkage bars is the time
after demolding (day 1). As shown in this figure, the inclusion of 0, 5, 10, 15 and 20% LF
after demolding (day 1). As shown in this figure, the inclusion of 0, 5, 10, 15 and 20% LF
increased the chemical shrinkage within the first 24 h. Thus, the formation of calcium
increased the chemical shrinkage within the first 24 h. Thus, the formation of calcium car-
carboaluminate resulting from the reaction between LF and C3 A in the cement increased
boaluminate resulting from the reaction between LF and C3A in the cement increased the
the total volume of the hydrate products [28,29,49,50]. For the longer curing period, it was
total volume
shown of the hydrate
that chemical shrinkage products [28,29,49,50].
kept going up as the For
curingthetime
longer curing period,
increased. it was
For example,
shown
at 1 day,that
the chemical
chemical shrinkage
shrinkage kept of thegoing
10% LF up replacement
as the curinglevel timewasincreased. For example,
about 619.5 µm/m.
This value rose to around 840.7 and 1239 µm/m at 10 and 45 days, respectively.619.5
at 1 day, the chemical shrinkage of the 10% LF replacement level was about µ m/m.
Therefore,
This value rose to around 840.7 and 1239 µ m/m at 10 and 45 days,
the reaction between cement particles and LF perpetuated with time. For the first 3 days, respectively. Therefore,
the chemical
the reaction between
shrinkage cement
valuesparticles and LF perpetuated
were approximately similar with time.
for all ForAt
mixes. the90first 3 days,
days, the
the chemical shrinkage values were approximately similar
chemical shrinkage of pastes with 0% LF attained a value of 1578.2 µm/m. This value for all mixes. At 90 days, the
chemical to
increased shrinkage
1961.7 µm/mof pastesat 5% with
LF 0%andLF thenattained
faintlyadropped
value ofwith 1578.2theµaddition
m/m. Thisofvalue
10% LF in-
creased to 1961.7 µ m/m at 5% LF and then faintly dropped
(1917.4 µm/m). After this slight decline, the chemical shrinkage went up to the optimumwith the addition of 10% LF
(1917.4 µ m/m). After this slight decline, the chemical shrinkage
value of 2861.4 µm/m at 15% LF. For an inclusion of 20%, the chemical shrinkage displayed went up to the optimum
avalue
sharpofdrop
2861.4 andµ m/m at 15%
reached LF. For
a value ofan inclusion
1770 µm/m.ofThis 20%,maythe chemical
be explainedshrinkage
by thedisplayed
fact that
a sharp drop and reached a value of 1770 µ m/m. This
with a high amount of LF (>15%), as the curing time increased, the formation may be explained by the fact that
of calcium
with a high amount
carboaluminate hydrate of LF (˃15%),
could as the
consume CH. curing
Thus,time increased,effect
the chemical the formation
of LF could ofincrease
calcium
carboaluminate
the solid volumehydrate could consume
of hydration productsCH. Thus, the
(external chemical effect
expansion), whichofreduced
LF couldthe increase
total
the solid
system volume(chemical
volume of hydration products
shrinkage) (external
[19]. expansion),
Additionally, which reduced
LF would mainly show the total sys-
a filler
tem volume
effect (chemical
which refined theshrinkage)
pore structure[19]. Additionally,
and reduced the LF porosity
would mainly of theshow
cement a filler
[23].effect
The
which refined of
incorporation thediverse
pore structure
percentagesand reduced the porosity
of LF enhanced of the cement
the chemical [23]. The
shrinkage incor-
of pastes.
poration
This of can
finding diverse percentages
be explained of LF enhanced
as follows: the chemical
(a) Considering the factshrinkage
that chemicalof pastes.
shrinkageThis
isfinding
a direct canresult
be explained as follows:
of the hydration (a) Considering
processes, the cementthe fact that chemical
hydration shrinkage
acceleration due istoa
direct
the result of
presence ofthe
LF hydration
increases the processes,
chemical theshrinkage
cement hydration
[27], andacceleration
(b) LF withdue to the
a fine pres-
particle
enceafford
size of LF nucleation
increases the chemical
sites shrinkage
for hydration [27], and
products (b) LF with accelerate
to precipitate, a fine particle size afford
the hydration
process
nucleation andsites
increase the hydration
for hydration degree
products of the cement
to precipitate, [23]. the hydration process and
accelerate
increase the hydration degree of the cement [23].
 Buildings 2021, 11, x FOR PEER REVIEW
Buildings 2021, 11, 366 7 of 17

Curing duration (days)

0 10 20 30 40 50 60 70 80 90
0

-500
Chemical shrinkage (µm/m)
-1000

-1500
P0%
-2000
P5%
-2500 P10%
P15%
-3000
P20%
-3500
Figure 6. Chemical shrinkage of pastes with different percentages of LF over 90 days.
Figure 6. Chemical shrinkage of pastes with different percentages of LF over 90 days.
3.2. Drying Shrinkage
3.2.
The results forDrying Shrinkage
the drying shrinkage for all paste specimens are presented in Figure 7.
The incorporation of 0%results
The LF displayed
for theexpansion for the firstfor
drying shrinkage fewall
days. This
paste phenomenon
specimens are presen
was not expected, but this small expansion has been observed by other studies
7. The incorporation of 0% LF displayed expansion for the first few [51]. Asdays. Th
displayed, all plots show similar trends. Drying shrinkage values increased as the curing
non was not expected, but this small expansion has been observed by other
time went up. For example, at 1 day, the drying shrinkage of the 5% LF replacement
As displayed, all plots show similar trends. Drying shrinkage values increas
was 0 µm/m. This value went up to a value of 900 and 1275 µm/m at 15 and 45 days,
respectively. ing
The time went up.
mechanism For example,
of long-term dryingat 1shrinkage
day, thecan
drying shrinkage
be well of the
explained by 5% LF
Buildings 2021, 11, xthe disjoining
FOR was 0 µ m/m.
pressure,
PEER REVIEW This
which value went
is relevant updrying
to the to a value of 900
shrinkage and 1275
in paste µ m/m
[52–55]. Thisat 15 and
spectively. The mechanism of long-term drying shrinkage can
disjoining pressure existing between capillary pores could result in the contraction of the be well exp
solid body. disjoining pressure, which is relevant to the drying shrinkage in paste [52–
joining pressure existing between capillary pores could result in the contr
solid body. Curing duration (days)
0 1 0It was2 noticed
0 3 0 as well
4 0 that5the
0 drying
6 0 shrinkage
70 8 0rose 9as0 the LF content i
1000 example, at 90 days, the inclusion of 0% LF achieved a value of 950 µ m/m. Th
sequently P0% P5% P10%the highest
P15% value
P20%of 1900 µ m/m with the add
Drying shrinkage (µm/m)

rose until achieving

500
LF. The reason for this elevation may be attributed to the drop of Young’s m
0 paste as well as the difference in capillary pore structure connectivity, which
moisture escape [56–59].
-500 It can be stated that the w/b ratio can play a significant role in drying s
velopment. The paste in this case will be more porous with more connectivi
-1000 increase the rate of water evaporation, thus increasing the drying shrinkage
[17,56,60,61]. The addition of the LF content tended to amplify the drying sh
-1500
was due to the strong impact of an internal reaction which enhanced the cohe
-2000 the cement and LF [62]. Hence, this opposite phenomenon encourages disr
compaction of the paste, resulting in a higher amount of entrapped voids, w
-2500 greater drying shrinkage [62].
Figure 7. Drying shrinkage of pastes with different percentages of LF over 90 days.
Figure 7. Drying shrinkage of pastes with different percentages of LF over 90 days.
It was noticed as well that the drying shrinkage rose as the LF content increased. For
example, at 90 days, the inclusion of 0% LF achieved a value of 950 µm/m. This value
3.3. Autogenous Shrinkage
subsequently rose until achieving the highest value of 1900 µm/m with the addition of
20% LF. The reasonFigure
for this8 displays
elevationthe
mayautogenous shrinkage
be attributed to the for
dropvarious pastesmodulus
of Young’s during the first 9
of curing. Generally, there was a tendency to have small expansion during the fir
days of curing, and thereafter autogenous shrinkage started to occur. As shown, t
togenous shrinkage was influenced by the LF content. At 90 days, the autogenous s
age for the 0% addition was 1100 µ m/m. This value went up and reached the opt
Buildings 2021, 11, 366 8 of 17

of the paste as well as the difference in capillary pore structure connectivity, which led to
easier moisture escape [56–59].
It can be stated that the w/b ratio can play a significant role in drying shrinkage
development. The paste in this case will be more porous with more connectivity, which
can increase the rate of water evaporation, thus increasing the drying shrinkage of the
paste [17,56,60,61]. The addition of the LF content tended to amplify the drying shrinkage.
This was due to the strong impact of an internal reaction which enhanced the cohesion
between the cement and LF [62]. Hence, this opposite phenomenon encourages disruption
in the compaction of the paste, resulting in a higher amount of entrapped voids, which
leads to greater drying shrinkage [62].

3.3. Autogenous Shrinkage

Figure 8 displays the autogenous shrinkage for various pastes during the first 90 days
of curing. Generally, there was a tendency to have small expansion during the first few days
of curing, and thereafter autogenous shrinkage started to occur. As shown, the autogenous
shrinkage was influenced by the LF content. At 90 days, the autogenous shrinkage for
the 0% addition was 1100 µm/m. This value went up and reached the optimum value of
1650 µm/m with the incorporation of 10% LF. After this sharp increase, the autogenous
shrinkage values dropped with the addition of 15 and 20% LF. This can be explained by the
fact that LF fills the porous structures and produces higher capillary forces, which increases
the self-desiccation during cement hydration. Moreover, for replacements above 10% LF,
due to the internal curing effect, the released water from specimens with 15 and 20%
Buildings 2021, 11, x FOR PEER REVIEW
LF
9 of 18
can fill the emptied pore and leads to a reduction in the degree of self-desiccation and
autogenous shrinkage [7,63–67].

Curing duration (days)

0 10 20 30 40 50 60 70 80 90
1000
P0% P5% P10% P15% P20%
Autogenous shrinkage (µm/m)

500

-500

-1000

-1500

-2000
Autogenousshrinkage
Figure8.8.Autogenous
Figure shrinkageofofpastes
pasteswith
withdifferent
differentpercentages
percentagesof
ofLF.
LF.

It can be also detected that with the rising of curing time, the autogenous shrinkage
3.4. Expansion
will definitely rise. For example, at 1 day, the autogenous shrinkage value for 5% LF
was The expansion
0 µm/m. results
This value fortothe
rose pasteofspecimens
a value 450 and 900with
µm/m different percentages
at 10 and of LF are
45 days, respectively.
presented
This was due in Figure 9. The paste
to the pozzolanic specimens
reactions displayed
of the LF, which continuous expansion
led to an increase from zero
in autogenous
time until 90 days. As
shrinkage [26,63,68,69]. shown in this plot, there was a logical variation in the expansion
results when incorporating the LF content. For example, at 90 days, the expansion value
3.4.the
for Expansion
0% LF replacement was 2000 µ m/m. This value rapidly decreased to a minimum
value The
of 1200 µ m/m with
expansion the for
results addition of 10%
the paste LF. Afterwith
specimens thisdifferent
sharp decrease, the expansion
percentages of LF are
value rose in
presented again up9.toThe
Figure 2100 µ m/m
paste and 2150
specimens µ m/m with
displayed the inclusion
continuous of 15from
expansion and zero
20% time
LF,
respectively.
until 90 days.Therefore,
As shownadding 15% LF
in this plot, and
there above
was enhanced
a logical the in
variation self-desiccation
the expansiondue to
results
hydration. In particular, the curing time had an obvious effect on the expansion. The ex-
pansion increased as the curing time rose for all percentages. For example, at 1 day, the
expansion of the 5% LF replacement was 0 µ m/m. This value went up to a value of 800 and
1400 µ m/m at 10 and 45 days, respectively. Moreover, as the curing time increased, swell-
ing in the bars rose much more for the pastes with high LF contents (15 and 20%) than in
Buildings 2021, 11, 366 9 of 17

when incorporating the LF content. For example, at 90 days, the expansion value for the
0% LF replacement was 2000 µm/m. This value rapidly decreased to a minimum value of
1200 µm/m with the addition of 10% LF. After this sharp decrease, the expansion value rose
again up to 2100 µm/m and 2150 µm/m with the inclusion of 15 and 20% LF, respectively.
Therefore, adding 15% LF and above enhanced the self-desiccation due to hydration. In
particular, the curing time had an obvious effect on the expansion. The expansion increased
as the curing time rose for all percentages. For example, at 1 day, the expansion of the
5% LF replacement was 0 µm/m. This value went up to a value of 800 and 1400 µm/m at
10 and 45 days, respectively. Moreover, as the curing time increased, swelling in the bars
rose much more for the pastes with high LF contents (15 and 20%) than in specimens with
low LF contents. This was due to the hydrate products (monocarboaluminate and hemi
or mono-carbonate) [49] that were formed at high LF contents being able to absorb more
water and swell more than pastes with low LF contents [19,26]. Furthermore, it could be a
result of the changes in phase composition within the hydrate network. As the CH content
Buildings 2021, 11, x FOR PEER
in theREVIEW
system reduced due to the addition of the LF content, the calcium aluminate was 10 of 1

gradually replaced by carboaluminate, which has a lower density than calcium aluminate,
providing an extra contribution to the expansion process [19,49].

2500
P0% P5% P10% P15% P20%
Expansion (µm/m)

2000

1500

1000

500

0
0 10 20 30 40 50 60 70 80 90
Curing duration ( days)
Figure 9. Expansion of pastes with different percentages of LF.
Figure 9. Expansion of pastes with different percentages of LF.
3.5. Comparison between Chemical, Autogenous and Drying Shrinkage and Expansion
Figures
3.5. 10–14 present
Comparison the length
between change
Chemical, (chemical,and
Autogenous drying and
Drying autogenous
Shrinkage shrinkage
and Expansion
and expansion) of pastes for 0, 5, 10, 15 and 20% LF, respectively, over 90 days. By
Figures 10–14 present the length change (chemical, drying and autogenous shrinkage
comparing the development of shrinkage over 90 days, it seems that the chemical shrinkage
and expansion) of pastes for 0, 5, 10, 15 and 20% LF, respectively, over 90 days. By com
values were the highest among all other shrinkages. Likewise, the inclusion of LF achieved
paring the development of shrinkage over 90 days, it seems that the chemical shrinkage
a noticeable enhancement in shrinkage. According to the results illustrated in these figures,
values were the highest among all other shrinkages. Likewise, the inclusion of LF achieved
it appears that the drying shrinkage was clearly greater than the autogenous shrinkage.
a noticeable enhancement in shrinkage. According to the results illustrated in these fig
This is well observed in Figure 13. The results are to be expected given that autogenous
ures, it appears that the drying shrinkage was clearly greater than the autogenous shrink
shrinkage is caused by self-desiccation in paste as water is consumed during the hydration
age. This is well observed in Figure 13. The results are to be expected given that autoge
process. This generally occurs within the early days of casting the paste. However, drying
nous shrinkage is caused by self-desiccation in paste as water is consumed during the
shrinkage is the reduction in paste volume caused by the loss of water during the drying
hydration process. This generally occurs within the early days of casting the paste. How
mechanism, and this continues perhaps for years after paste curing [63–66]. Additionally,
ever,values
all shrinkage dryingincreased
shrinkageas is the
the reduction
curing timein went
paste up.
volume caused
Adding byLF
15% theattained
loss of water
the during
maximum thechemical
drying mechanism, and this continues
shrinkage. However, perhaps
the inclusion forLFyears
of 10% afterLF
and 20% paste curing [63–66]
exhibited
the highest autogenous and drying shrinkage, respectively. Concerning the expansion, 15% LF
Additionally, all shrinkage values increased as the curing time went up. Adding
there wasattained the maximum
a decrease between 0 chemical
and 10% shrinkage.
LF. BeyondHowever,
this level,the inclusion
there was anofincrease
10% LF and
in 20% LF
shrinkage, with a maximum value of 2150 µm/m occurring at the 20% replacement level. the ex
exhibited the highest autogenous and drying shrinkage, respectively. Concerning
pansion, there was a decrease between 0 and 10% LF. Beyond this level, there was an
increase in shrinkage, with a maximum value of 2150 µ m/m occurring at the 20% replace
ment level.
Buildings 2021, 11, 366 10 of 17

3.6. Relationships between Different Length Change Parameters

As mentioned in previous studies, the total chemical shrinkage is the sum of the exter-
nal and internal volume changes [8,70,71]. In general, at early ages, the external dimensions
of a paste can either drop due to self-desiccation (i.e., autogenous shrinkage) or to external
drying (i.e., drying shrinkage) or rise due to expansion. The internal volume change repre-
Buildings 2021, 11, x FOR PEER REVIEW
sents the chemical shrinkage [3]. On the other side, some authors define chemical shrinkage
Buildings 2021, 11, xin
FOR PEERof
terms REVIEW
the total chemical shrinkage and external chemical shrinkage [5,9]. After the 1
paste becomes stiff and can resist a contracting force, the external chemical shrinkage is
equal to the total chemical shrinkage.
Curing duration ( days)
0 10 20 30
Curing 40 50( days)
duration 60 70 80 90
25000 10 20 30 40 50 60 70 80 90
2500
1500
Length change (µm/m)

1500
Length change (µm/m)

500
500
-500
-500
-1500
-1500
-2500
Chemical shrinkage Drying shrinkage
-2500 Autogenous shrinkage Expansion
-3500 Chemical shrinkage Drying shrinkage
Autogenous shrinkage Expansion
-3500
Figure 10. Length change ofFigure
pastes10. Length
with change of pastes with 0% LF.
0% LF.
Figure 10. Length change of pastes with 0% LF.
Curing duration (days)
0 10 20 30
Curing 40 5 0(days)6 0
duration 70 80 90
25000 10 20 30 40 50 60 70 80 90
2500
1500
Length change (µm/m)

1500
Length change (µm/m)

500
500
-500
-500
-1500
-1500
-2500
Chemical shrinkage Drying shrinkage
-2500 Autogenous shrinkage Expansion
Chemical shrinkage Drying shrinkage
-3500
Autogenous shrinkage Expansion
-350011. Length change ofFigure
Figure pastes11.
with 5% LF.
Length change of pastes with 5% LF.
Figure 11. Length change of pastes with 5% LF.
 Buildings 2021, 11, x FOR PEER REVIEW
Buildings 2021, 11, Buildings
366 2021, 11, x FOR PEER REVIEW 11 of 17

Curingduration
Curing duration(days)
(days)
00 1 01 0 2 02 0 3 03 0 4 04 0 5 05 0 6 06 0 7 07 0 8 08 0 9 09 0
2500
2500

1500
1500

Length change (µm/m)

Length change (µm/m)
500
500

-500
-500

-1500
-1500

-2500
-2500 Chemical
Chemical shrinkage
shrinkage Drying
Drying shrinkage
shrinkage
Autogenous shrinkage
Autogenous shrinkage Expansion
Expansion
-3500
-3500
Figure
Figure 12. Length changeFigure
of 12.12.
pastes Length
with 10%
Length change
LF. of of
change pastes
pastes with
with 10%
10% LF.
LF.

Curingduration
Curing duration(days)
(days)
00 1 01 0 2 02 0 3 03 0 4 04 0 5 05 0 6 06 0 7 07 0 8 08 0 9 09 0
2500
2500

1500
1500
Length change (µm/m)
Length change (µm/m)

500
500

-500
-500

-1500
-1500

-2500
-2500
Chemical
Chemical shrinkage
shrinkage Drying
Drying shrinkage
shrinkage
Autogenous shrinkage
Autogenous shrinkage Expansion
Expansion
-3500
-3500
Figure 13. Length change of pastes13.
Figure with 15% change
Length LF.
Figure 13. Length change of of pastes
pastes with
with 15%
15% LF.
LF.
Buildings 2021, 11, 366Buildings 2021, 11, x FOR PEER REVIEW 12 of 17

Curing duration (days)

0 10 20 30 40 50 60 70 80 90
2500

1500
Length change (µm/m)
500

-500

-1500

-2500 Chemical shrinkage Drying shrinkage

Autogenous shrinkage Expansion
-3500
Figure 14. Length change ofFigure
pastes14.
withLength change of pastes with 20% LF.
20% LF.

The relationships between chemical

3.6. Relationships between shrinkage
Differentand the other
Length length
Change change parameters—
Parameters
autogenous shrinkage, drying shrinkage and expansion at different curing ages (1, 7, 28 and
As mentioned in previous studies, the total chemical shrinkage is the sum o
90 days)—are illustrated in Figures 15–17, respectively. As shown in Figure 15, a positive
ternal and internal volume changes [8,70,71]. In general, at early ages, the externa
relation existed between chemical shrinkage and autogenous shrinkage. This plot draws a
sions of a paste can either drop due to self-desiccation (i.e., autogenous shrinka
linear relationship, with a coefficient of determination R2 of 0.89, 0,89, 0.73, 0.96 and 0.66
external drying (i.e., drying shrinkage) or rise due to expansion. The internal
for 0, 5, 10, 15 and 20% LF, respectively. This means that during the hydration process and
change represents the chemical shrinkage [3]. On the other side, some author
after setting started, chemical shrinkage did not occur spontaneously, since it was delayed
chemical shrinkage in terms of the total chemical shrinkage and external chemica
by the rigidity of the paste itself [3]. Hence, water took its place in the finesse pores of
Buildings 2021, 11, x FOR PEER REVIEW age [5,9]. After the paste becomes stiff and can resist a contracting force, the extern
the cement paste. As the hydration process progressed, the volume of the water in the
ical shrinkage is equal to the total chemical shrinkage.
pores dropped. Thus, a process known as self-desiccation took place and led to creating
The relationships between chemical shrinkage and the other length change
autogenous shrinkage. Additionally, and before the initial setting of the paste, the capillary
ters—autogenous notshrinkage, drying shrinkageasand
theexpansion atthe
different curingi
forces were almostshrinkage
negligible.did Thus, take place.
chemical Furthermore,
shrinkage was essentially amount
the onlyofmotivator
LF content
7, 28 and 90 days)—are illustrated in Figures 15–17,
(above 15% LF), the less shrinkage and expansion would always exist.
for autogenous shrinkage. respectively. As shown in F
a positive relation existed between chemical shrinkage and autogenous shrinka
plot draws a linear relationship, with a coefficient of determination R2 of 0.89, 0
Chemical shrinkage (µm/m)
0.96 and 0.66 for 0, 5, 10, 15 and 20% LF, respectively. This means that during the h
- 3 5 0 0 process
- 3 0 0 0 and- 2after
5 0 0 setting
- 2 0 0started,
0 - 1 5chemical
0 0 - 1 shrinkage
000 - 5 0did
0 not occur
0 spontaneously
0 was delayed by the rigidity of the paste itself [3]. Hence, water took its place in th
pores yof= 0.8x
the +cement
16.19 paste. As the hydration process progressed, the volume of t
Autogenous shrinkage (µm/m)

-200 P0%
in the pores dropped. Thus, a process known as self-desiccation took place an
R²= 0.89
-400
creating autogenous shrinkage. Additionally, and before the initial setting of th
P5% y = 0.87x + 434.2
-600 the capillary forces were almost negligible. Thus, chemical shrinkage was essen
R²= 0.89
-800 only motivator for autogenous shrinkage.
P10%Similarly, the relation between chemical shrinkage and drying shrinkage
y = 1.1x + 137.81
-1000
portional.R²The = 0.73coefficient of determination R2 was 0.8, 0.67, 0.69, 0.92 and 0.89 fo
-1200 15 and 20% LF, respectively (Figure 16). This indicates that chemical shrinkage i
P15% y = increase
0.53x + 259.7
-1400 with the in drying shrinkage. Chemical shrinkage occurred before th
R²= 0.96
-1600 time of the paste while drying shrinkage took place after the setting time or w
P20%
paste started
y = 0.87x to harden. Thus, chemical shrinkage was a basic contributor fo
+ 115.7
-1800
shrinkage.R² = 0.66
Furthermore, the driving force of drying shrinkage was the loss of
-2000 resulting from the self-desiccation in the cement paste [26].
There was
Figure 15. Correlation between a negative
chemical shrinkage linear
andrelation between
autogenous chemical
shrinkage shrinkage and expans
for pastes.
Figure 15. Correlation
ure 17). This between chemical
negative shrinkage
relation and autogenous
indicates that as the shrinkage
chemical for pastes. values in
shrinkage
the expansion of the paste dropped. In fact, when the bars were cured in water, w
self-desiccation Chemical
existed, theshrinkage
bars exhibited
(µm/m)continuous expansion over time. T
-3500 -3000 -2500 -2000 -1500 -1000 -500 0
500
µm/m)

0
P0% y = 0.92x + 312.2
 -1400

Autogen
R²= 0.96
-1600
P20% y = 0.87x + 115.7
-1800 R²= 0.66
-2000
Buildings 2021, 11, 366 13 of 17

Figure 15. Correlation between chemical shrinkage and autogenous shrinkage for pastes.

Chemical shrinkage (µm/m)

-3500 -3000 -2500 -2000 -1500 -1000 -500 0
500

Drying shrinkage (µm/m)

0
P0% y = 0.92x + 312.2
R²= 0.8
-500
P5% y = 0.93x + 241.4
R²= 0.67
-1000
P10% y = 1x + 85.5
R²= 0.69
-1500
P15% y = 0.78x + 322.7
R²= 0.92
-2000
y = 1.41x + 645.8
Buildings 2021, 11, x FOR PEER REVIEW P20% R²= 0.89
-2500
Figure 16. Correlation
Figure between
16. Correlation chemical
between shrinkage
chemical and drying
shrinkage and shrinkage for pastes.
drying shrinkage for pastes.

2500

2000
Expansion (µm/m)

1500
P0% y = -1.57x - 204.11
R²= 0.95
P5% y = -1.25x - 528.12
1000 R²= 0.85
y = -0.69x - 43.63
P10%
R²= 0.71
P15% y = -0.9x - 297.45
500
R²= 0.87
P20% y = -1.52x - 569.69
R²= 0.86
0
-3500 -3000 -2500 -2000 -1500 -1000 -500 0
Chemical shrinkage (µm/m)
Figure 17. Correlation between chemical
Figure 17. Correlation betweenshrinkage
chemical and expansion
shrinkage and for pastes. for pastes.
expansion

Similarly, 4.
theConclusions
relation between chemical shrinkage and drying shrinkage was propor-
tional. The coefficient of determination R2 was 0.8, 0.67, 0.69, 0.92 and 0.89 for 0, 5, 10,
This paper discusses the volume stability of paste incorporating limestone fin
15 and 20% LF, respectively (Figure 16). This indicates that chemical shrinkage increased
cement replacement. The volume stability included three types of shrinkage—che
with the increase in drying shrinkage. Chemical shrinkage occurred before the setting time
autogenous and drying—and expansion. Based on the results obtained in this e
of the paste while drying shrinkage took place after the setting time or when the paste
mental work, the following conclusions can be made:
started to harden. Thus, chemical shrinkage was a basic contributor for drying shrinkage.
Furthermore, the driving
Chemical
forceshrinkage
of drying increased
shrinkage for
wassubstitutions levels between
the loss of moisture resulting0 from
and 15% LF,
the self-desiccation it
inachieved
the cement thepaste
highest value of 2861.4 µ m/m at 90 days. Beyond 15% LF substi
[26].
the chemical
There was a negative linearshrinkage
relation decreased.
between chemical shrinkage and expansion

(Figure 17). This negative relation indicates that asasthe
Drying shrinkage increased thechemical
LF content in the paste
shrinkage valuesincreased.
increased,At 90 da
the expansion of the maximum drying In
paste dropped. shrinkage
fact, whenvalue
theof 1900
bars µ m/m
were wasinachieved
cured for 20% LF re
water, where
ment. the bars exhibited continuous expansion over time. Therefore,
no self-desiccation existed,
shrinkage did not take
The length
place. change (autogenous
Furthermore, as the shrinkage)
amount of showed positiveincreased
the LF content values (i.e., expa
(above 15% LF), theforlessthe first fewand
shrinkage days (7 days)would
expansion for all always
replacements
exist. except for 10% LF replace
After this period, all replacements showed contraction. Autogenous shrinka
creased between 0 and 10% LF, where it achieved the highest value of 1650 µ
90 days followed by a sharp drop for compositions above 10% LF.
 The expansion values for the paste specimens showed a slight decrease for re
ments between 0 and 10% LF. Above 10% LF, there was sharp increase in expa
and the highest value of 2150 µ m/m was achieved for the paste with 20% LF.
 A positive correlation existed between chemical shrinkage and both autogeno
drying shrinkage. However, a negative correlation occurred between ch
Buildings 2021, 11, 366 14 of 17

4. Conclusions
This paper discusses the volume stability of paste incorporating limestone fines as a
cement replacement. The volume stability included three types of shrinkage—chemical,
autogenous and drying—and expansion. Based on the results obtained in this experimental
work, the following conclusions can be made:
• Chemical shrinkage increased for substitutions levels between 0 and 15% LF, where it
achieved the highest value of 2861.4 µm/m at 90 days. Beyond 15% LF substitution,
the chemical shrinkage decreased.
• Drying shrinkage increased as the LF content in the paste increased. At 90 days, the
maximum drying shrinkage value of 1900 µm/m was achieved for 20% LF replacement.
• The length change (autogenous shrinkage) showed positive values (i.e., expansion) for
the first few days (7 days) for all replacements except for 10% LF replacement. After
this period, all replacements showed contraction. Autogenous shrinkage increased
between 0 and 10% LF, where it achieved the highest value of 1650 µm/m at 90 days
followed by a sharp drop for compositions above 10% LF.
• The expansion values for the paste specimens showed a slight decrease for replace-
ments between 0 and 10% LF. Above 10% LF, there was sharp increase in expansion,
and the highest value of 2150 µm/m was achieved for the paste with 20% LF.
• A positive correlation existed between chemical shrinkage and both autogenous
and drying shrinkage. However, a negative correlation occurred between chemical
shrinkage and expansion.

Author Contributions: Conceptualization, J.K.; methodology, R.R.; formal analysis, R.R.; writing—
original draft preparation, R.R. and H.G.; writing-review and editing, J.K., H.G. and A.E.; supervision,
J.K. and A.E.; project administration, H.G. All authors have read and agreed to the published version
of the manuscript.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Data sharing is not applicable to this article.
Conflicts of Interest: The authors declare no conflict of interest.

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