Journal of Building Engineering 46 (2022) 103750

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Journal of Building Engineering

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Effect of nano-silica dispersed at different temperatures on the

properties of cement-based materials
Haibao Liu a, Qiuyi Li b, *, Songyuan Ni b, Liang Wang b, Gongbing Yue b,
Yuanxin Guo b
a
School of Civil Engineering, Qingdao University of Technology, Qingdao, 266033, China
b
School of Architectural Engineering, Qingdao Agricultural University, Qingdao, 266109, China

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

Keywords: The influence of nano-silica (NS) on the performance of cement is largely dependent on the de­
Nano-silica gree of dispersion. This study aims to clarify the influence of NS at different dispersion temper­
Ultrasonication atures on the properties, such as the hydration and hardening, of cement. The optimum dispersion
Hydration reaction temperature of NS was determined by measuring the particle-size distribution, hydration heat,
Dispersion temperature and mechanical strength. The microstructure and morphology of cement pastes and the content of
Cement
hydration products were studied to evaluate the effect of NS at different dispersion temperatures
on the properties of cement. The results indicated that the higher the temperature of NS
dispersion, the smaller the particles of NS aggregations. However, the higher temperature made
NS agglomerate more easily in the cement paste. The average particle size of NS in the extractive
solution of cement was the smallest, and the increase in hydration degree showed that the
improvement in NS on the properties of cement was greatest when the dispersion temperature
was 10 ◦ C. The 3d- and 28d-compressive strengths of the cement paste were increased by 22%
and 25%, respectively.

1. Introduction
Nanomaterials have many advantages and have been innovatively employed in the field of cement-based materials. For example,
carbon nanotubes and nano-graphene are used to ameliorate the shrinkage fracture performance of concrete [1–4]; nano-TiO2 is
incorporated into underground parking mortar for the photocatalytic treatment of automobile exhaust [5]. Among the nanomaterials,
nano-silica (NS) has been widely used in cementitious materials owing to its excellent performance advantages [6–11].
NS can react with calcium hydroxide (CH) in the secondary hydration reaction in a pozzolanic reaction, greatly improving the
mechanical strength and durability of cement at an appropriate amount of NS [12,13]. Said et al. [14] [][][]showed that the 28d-me­
chanical strength of concrete increased by 36% at 1 wt% NS addition. The 28d-mechanical strength of a mortar could be increased by
212% by adding 3 wt% of NS [15]. Moreover, many studies have shown that the seeding effect of NS can be more effective when it is
dispersed well. This phenomenon implies that NS can promote the hydration reaction of cement-based materials. The pozzolanic
activity of NS increases cement hydration, and the calcium silicate hydrate formed by hydration can effectively fill the micro-cracks
and pores of concrete and improves the mechanical properties and durability of concrete [16–19].
Although many studies have reported that NS can improve the properties of cementitious materials, challenges remain in practical

* Corresponding author.
E-mail address: lqyyxn@163.com (Q. Li).

https://doi.org/10.1016/j.jobe.2021.103750
Received 24 September 2021; Received in revised form 24 November 2021; Accepted 24 November 2021
Available online 1 December 2021
2352-7102/© 2021 Elsevier Ltd. All rights reserved.
H. Liu et al. Journal of Building Engineering 46 (2022) 103750

Table 1
Mineral composition of cement and NS by XRF, wt.%.

Chemical composition CaO SiO2 Al2O3 Fe2O3 SO3 MgO TiO2 Others

P⋅O 42.5 61.7 20.9 6.4 3.8 2.6 1.73 0.4 2.47
Nano-silica / 99.9 / / / / 0.1

applications. When NS is mixed into a cement paste, its particles with large surface energy easily form aggregates in high-pH and
complex ionic environments. The aggregates can lead to cement-based materials with poor mechanical properties [20–22]. Kong et al.
[23]reported that colloidal silica plays a better role in improving the properties of cement than NS. However, the aggregates in the
cement paste with colloidal silica are larger than that of NS, weakening the improvement of cement properties by colloidal silica.
Improper dispersion aggravate the agglomeration of NS, and the bonding strength of hydrated calcium silicate gel formed by NS
agglomeration decreases [24,25]. Moreover, the order of polycarboxylate superplasticizer (PCE) addition significantly influences the
mechanical strength of the cement paste [26]. In addition, according to nucleation theory, the seed effect is significantly weakened
when the amount of NS agglomeration is increased [27–29].
Nowadays, nanomaterial dispersion methods are mainly through chemical and physical means. Chemical dispersion includes
grafting functional groups onto nano-molecular particles and dispersing them with chemical dispersants [27,30]. A new type of
superplasticizer was synthesized and then grafted onto the surface of NS to prevent its agglomeration. However, different functional
groups only affect specific nanomaterials. Physical dispersion includes ultrasonic dispersion and mechanical stirring. Mechanical
stirring is the most commonly used dispersion method; however, it cannot eliminate agglomerations in nanomaterials effectively.
Ultrasonic dispersion has been widely used in laboratory and production applications because of its good dispersion effect. During
ultrasonication, high-frequency mechanical vibrations can produce microbubbles in NS agglomerates, which grow into cavitated
bubbles.
The high pressure and huge impact force generated by ultrasonic waves break the large agglomerates into small particles, thus
achieving the dispersion of nanomaterial agglomerates [31–33]. Ultrasonic power and time have been used in many studies about
nano-material dispersion [34–38]. In ultrasonic dispersion, studies are more concerned about the output power and duration, which
tends to lead to a misunderstanding: the higher the output power and the longer the duration, the better the dispersion effect of
nanomaterials. Some studies [36,39–41] have shown that inappropriate ultrasonic energies may lead to the re-agglomeration of NS
particles, resulting in failed nanomaterial dispersion.
Ultrasonic energy is produced through the vibration of the amplitude variation rod, where the energy is mainly distributed in three
parts. One part of the energy is converted into ineffective mechanical vibration of the rod, another is converted into thermal energy
that increases the temperature of the dispersion, and the remaining part is used to fragment and disperse nanoparticle agglomeration.
This energy distribution may not have a proportional relationship; that is, the distribution relationship cannot be analyzed quanti­
tatively. At the same time, in the ultrasonic dispersion research on nano-silica and other materials, there are few studies on the effect of
temperature on the dispersion effect and the use effect in the dispersion experiment, clarifying the influence of temperature on
dispersion on dispersion during ultrasonication has a good research potential.
In this study, the effect of NS on the properties of cement-based materials under different dispersion temperatures was studied. The
optimum temperature during ultrasonic dispersion and its effect on cement-based materials are largely dependent on the degree of
agglomeration of nanomaterials in the cement solution, hydration heat, and mechanical strength of cement pastes. The phase contents
of CH and the Ca/Si atom ratio in hydrated calcium silicate gel were used to assess the effect of NS on the performance of the cement
materials.

2. Materials and methods

2.1. Raw materials
Ordinary Portland cement (P⋅O 42.5 grade) was produced by Qingdao Shanshui Cement Co., Ltd., which fulfills the Chinese na­
tional standard GB/T 17671-2020, was used in the study. NS powder is produced by Shanghai Aladdin Materials Co., Ltd., and its
particle size ranges from 20 nm to 50 nm. The main chemical compositions of the cementitious material and NS are shown in Table 1.
Distilled water was used for the experiment.

2.2. Sample preparation

2.2.1. Dispersion of NS in distilled water
Ultrasonic energy is determined by ultrasonic power and time. In general, the larger the output energy, the smaller the particle size
of the nanomaterials. However, this trend is not consistent. Since the ultrasonic energy is not absorbed completely by NS agglomerates,
part of it is converted into heat. The sample was placed in a constant-temperature tank during the experiment to clarify the effect of
solution temperature in the ultrasonic dispersion process. The temperature in the tank was maintained by an antifreeze attached to a
circulation system. The dispersion temperature was changed by adjusting the antifreeze temperature. The ultrasonic dispersion test
process is shown in Fig. 1.
In this experiment, distilled water (400 g) and NS powder (8 g, accounting for 2% of the weight of cement) were weighed and then
dispersed by ultrasonic waves. The ultrasonic powers were set to 200, 400, 600, and 800 W for 15 min. After the dispersion test, the
particle-size distribution and morphology were immediately characterized. Transmission electron microscopy (TEM) was used to

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Fig. 1. Schematic of the ultrasonic dispersion test.
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Table 2
Parameters used to prepare the cement samples.

Samples Cement (wt%) Nano-silica (wt%) Superplasticizer (wt%) Dispersion temperature(◦ C)

Control 98 2 1 No control
B1 98 2 1 10
B2 98 2 1 25
B3 98 2 1 40
B4 98 2 1 55

Table 3
Effect of output energies on particle size of NS.

Samples Power (W) Energy (kJ) Solution temperature after dispersion (◦ C) Mean Particle Size(nm)

Holding time

0h 24h 72h

A1 200 90 33 165 230 380

A2 400 180 35 150 203 345
A3 600 270 40 75 142 185
A4 800 360 43 68 120 223

characterize the morphology of the samples.

2.2.2. Dispersion of NS in cement solution

The distribution of NS in the cement paste was determined by extracting the supernatant of the cement solution. The supernatant
was extracted by mixing the NS dispersion with cement. The distilled water (mixed water) and NS were ultrasonically dispersed for 15
min at constant temperature (the temperatures were maintained at 10, 25, 40, and 55 ◦ C). Then, the dispersion and cement were mixed
in a ratio, s/c = 5 (s and c represent NS dispersion and cement, respectively). The mixture was then stirred quickly for 3 min using a
cement paste mixing machine, followed by centrifugation at 12,000 rpm for 5 min. Subsequently, the samples were collected
immediately to determine their particle-size distribution.

2.2.3. Cement pastes doped with NS

Studies have shown that the mixing order of materials may affect the addition effect of NS [26]. Herein, NS suspension was added
first, followed by superplasticizer. The parameters, Water/Cement = 0.5, NS (2 wt% of cement), and superplasticizer (1 wt% of
cement), were used to prepare cement pastes. The component information is presented in Table 2.
The experimental process of the cement pastes was as follows. All raw materials were mixed successively at low speed (60 rpm/
min) and high speed (120 rpm/min) for 90 s with an interval of 30 s. The sample was cast into a 20 mm × 20 mm × 20 mm mold,
demolded after 24 h, all samples were placed in a curing room with a temperature of 20 ± 1 ◦ C and a relative humidity of no less than
90% for 24 h, then demolded and cured in water until different ages.

2.3. Test methods

2.3.1. Heat of hydration
The hydration heat of the cement was tested using a microcalorimeter (TAM Air) under operation at 5–90 ◦ C. The hydration
temperature was measured using the adiabatic method. The recording time of the hydration heat of the cement samples lasted for 72 h.

2.3.2. Particle size distribution

NS was dispersed in distilled water and cement solution under specific conditions using a particle-size distribution analyzer
(Nicomp 380 N300, USA). It is necessary to clarify the influence of standing time on the dispersion effect of NS. Thus, the aggregate
particles of the NS dispersion were analyzed statistically after standing for 0, 24, and 72 h.

2.3.3. Microscopic morphology observation

The morphology of NS particles dispersed by ultrasonic waves in an anhydrous ethanol solution was analyzed using TEM
(JCM7000, Japan). When preparing the sample, the test solution was dropped on an aluminum foil, dried, and then and then tested.
A scanning electron microscope (SEM) (JSM-7500F, Japan) was used to observe the effect of NS on the microstructure of the
cement. The cement samples were sliced thin, placed in acetone for 10 h to terminate the hydration, and sprayed with gold. After the
above experiments were completed, SEM experiments were performed.

2.3.4. Compressive strength

An automatic electronic strength machine (DYE-300S, China) was used to test the compressive strength of the cement pastes. Three
20 mm × 20 mm × 20 mm specimens were tested at each target age.

2.3.5. Setting time

The Vicat needle test method specified in the Chinese national standard GB/T1346-2011 was employed to test the setting time of

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Fig. 2. Particle-size distribution of NS under different dispersion powers. Left for (a) 0 h, (b) 24 h, and (c) 72 h.
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Fig. 3. TEM images of NS at different ultrasonic dispersion powers. (a) 200 W, (b) 400 W, (c) 600 W, and (d) 800 W.

the cement slurry.

2.3.6. Analysis of hydration products

Differential thermal analysis of the hydration product was performed using a comprehensive thermal analyzer (Q600, USA) be­
tween 20 and 800 ◦ C at a heating and flow rate of 25 ◦ C/min and N2, respectively.

3. Results and discussions

3.1. Influence of ultrasonic output energy on particle size
Ultrasonic dispersion can rely on the high pressure generated by liquid cavitation that can break NS agglomerates into small
particles and disperse NS. The ultrasonic dispersion equipment can change the energy output for NS dispersion by adjusting the
dispersion time and power. To clarify the influence of ultrasonic power on the dispersion of NS particles, dispersion powers at 200,
400, 600, and 800 W were applied for 15 min with a working sequence of 3 s and an interval of 3 s, as shown in Table 3.
Normally, only a portion of the ultrasonic output energy can be used to break up the dispersed agglomerates of NS, while the rest of
the energy is converted into heat and mechanical vibration. When the dispersion energy showed an equal incremental change, the
dispersion temperature did not exhibit a corresponding linear change. This implies that the energy input to ultrasonic dispersion may
be disordered among the three energy transfer methods.
From Fig. 2, it can be seen that the average particle size decreased as the dispersion power increased. The average particle size at
200 W and 400 W was larger than that at 600 W and 800 W (160–190 nm vs. 60–80 nm). Meanwhile, the average particle size of NS in
the solution increased after the dispersion solution was left standing. Taking 600 W as an example, the average particle sizes of the NS
suspensions were 75, 142, and 185 nm after 0, 24, and 72 h of standing, respectively.
The TEM images of NS particles at different ultrasonic dispersion powers are shown in Fig. 3. The high ultrasonic power could break
up and disperse NS particles, resulting in a lower degree of agglomeration. Meanwhile, it can be observed that the mean particle sizes
of NS at 600 W were not significantly different from those at 800 W. The above results suggest that the most suitable ultrasonic
dispersion power for NS particles is 600 W, and 600 W was selected for the ultrasonic dispersion power in subsequent experiments.

3.2. Effect of dispersion temperature on the dispersion of NS particles

As shown in Fig. 4(a), the particle size of NS decreased with an increase in the dispersion temperature. When the temperature was
10 ◦ C (B1) and 25 ◦ C (B2), the average particle size of NS was larger than 40 ◦ C (B3) and 55 ◦ C (B4) (190–240 nm vs. 70–85 nm). TEM

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Fig. 4. Effect of dispersion temperature on dispersion of NS particles. (a) dispersed in distilled water and (b) supernatant of NS dispersion mixed with cement.

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Fig. 5. TEM images of NS at different dispersion temperatures. (a) 10 ◦ C, (b) 25 ◦ C, (c) 40 ◦ C, and (d) 55 ◦ C.

images of dispersed NS are shown in Fig. 5. The degree of agglomeration and bridging of NS decreased with an increase in the
dispersion temperature. According to the first law of thermodynamics [42], as the temperature of the solution increases, water
molecules and NS particles in the solution move disorderly at high speeds, making the NS particle agglomerates more likely to break up
and disperse under the effect of ultrasonic dispersion.
The particle-size distribution of NS in the supernatant after mixing NS dispersion with cement at different temperatures is shown in
Fig. 4(b). An interesting phenomenon is that the average particle size was significantly larger at 40 and 55 ◦ C than at 10 and 25 ◦ C
(6.5–7.3 μm vs. 1.9–2.6 μm), the opposite of the change in the particle-size distribution of NS in dispersions at different temperatures.
High temperatures make water molecules and NS particles more active. However, when the NS dispersion was fully mixed with cement
to create a high-pH multi-ion solution environment, the higher activity made NS particles prone to adsorption and particle agglom­
eration because of the high surface energy [43,44].
The above experimental phenomenon indicates that a higher dispersion temperature can effectively reduce the degree of particle
agglomeration in the NS dispersion, resulting in a smaller average particle size. However, when the NS dispersion was mixed with the
cement solution, the average particle size obtained by mixing the lower temperature NS dispersion was rather small, which means that
NS dispersion at lower temperatures has greater potential to improve the performance of cement.

3.3. Influence of different dispersion temperature on NS in cement paste

3.3.1. Cement hydration heat
The exothermic curves of cement hydration and cumulative heat of cement mixed with different NS dispersion temperatures are
shown in Fig. 6. The results showed that the addition of NS dispersion could accelerate the hydration rate and increase the cement
hydration exothermic peak [45,46]. The degree of promotion of the cement hydration rate became more significant with increased
dispersion temperature. This phenomenon may be caused by the nucleation effect of NS [16,26], which accelerates the rate of cement
hydration.
From the cement hydration exothermic peak and cumulative heat of hydration of the cement, it can be concluded that NS can
effectively improve the hydration degree of cement. The enhancement effect was best when the dispersion of NS was 10 ◦ C (B1) and
might be related to the degree of NS dispersion in the cement paste. When the NS dispersion was fully mixed with the cement to form a
high-pH, multi-ion solution environment, the NS dispersion at a high temperature made the NS particles more prone to particle
agglomeration and adsorption on the cement particle surface than that at low temperature. This phenomenon affected the hydration
process of cement and reduced the filling effect and nucleation of the NS. By contrast, the NS dispersion at low temperature reflected a
more stable state when mixed with cement paste, and the promotion effect on cement hydration was more significant.

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Fig. 6. Effect of NS dispersion at different temperatures on hydration heat release process. (a) heat flow curve and (b) cumulative heat curve of cement.

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Fig. 7. Growth rate of compressive strength and setting time.
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Fig. 8. CH content of cement paste samples with NS at different dispersion temperatures.

3.3.2. Compressive strength and setting time

The growth rate of the compressive strength of cement pastes mixed with NS dispersions at different temperatures is shown in Fig. 7
(a). Compared to the control group, the compressive strength of the cement paste mixed with NS was improved, with the greatest
increase in compressive strength at a dispersion temperature of 10 ◦ C (B1), which was similar to the change in the heat of hydration. A
lower dispersion temperature caused the NS particles to remain more stable and better dispersed in the cement paste after incorpo­
ration into the cement paste. Thus, the filling effect and nucleation of NS were more fully developed, which is undoubtedly beneficial
to mechanical strength. As shown in Fig. 7, the growth rate of the strength of the cement paste specimen became more pronounced
with increased curing age, which might be due to the secondary hydration reaction between NS and CH [16,26,30] to produce C–S–H
gel. The dense structure of cement paste had a positive influence on the development of compressive strength.
From Fig. 7, it can be clearly seen that the setting times of the samples with NS were shorter than those of the control group, and the
setting time of sample B1 was the longest, followed by B2, B3, and B4. This phenomenon is owing to the decrease in the dispersion of
NS in the cement paste and the free water wrapped by the aggregates of NS, which shortens the setting time [26,47].

3.3.3. Analysis of hydration products

Fig. 9 shows DTG curves of cement paste hydration products with the addition of NS. The decomposition temperature of CH on the
DTG curve occurred around 450–550 ◦ C, and the decomposition temperature of calcium carbonate was 650–800 ◦ C. The CH content in
each sample was calculated by the mass loss at 450–550 ◦ C, as shown in Fig. 8. The results showed that the CH content in the control
group was the highest among all samples, which was due to the consumption of the NS hydration reaction. Sample B1 (dispersion
temperature of 10 ◦ C) had the lowest content, followed by B2, B3, and B4. This trend is consistent with the change in the particle size
pattern of NS particles after dispersion in the cement solution. The above phenomenon indicates that the effect of NS incorporation was
related to its morphology in the cement slurry and that the well-dispersed NS has great potential for CH [43,48–50].
Related studies have shown that hydrated calcium silicate gel with a low Ca/Si atom ratio has a high degree of polymerization and
provides good mechanical strength to cement pastes [48]. Together with the morphology of the samples shown in Fig. 10, the Ca/Si
atomic ratios of all samples were statistically analyzed by energy-dispersive X-ray spectroscopy. As shown in Fig. 10, the Ca/Si atomic
ratio of all samples doped with NS was higher than that of the control group, and the lowest Ca/Si atom ratio of B1 was 1.91 and 1.66 at
3 and 28 d, respectively. This may be due to well-dispersed NS in the cement paste, resulting in the effective consumption of CH.

3.3.4. Microstructure analysis

The microstructures of the cement pastes mixed with NS dispersions at different temperatures are shown in Figs. 11 and 12. The
unconsumed NS agglomerations still existed at the curing age of 3 d. The NS agglomerations in B1 were the smallest, which means that
the dispersion of NS particles was the best. Thus, the filling effect, nucleation effect and pozzolanic reactivity of NS can be better
achieved. Combined with the results mentioned above, it can be safely concluded that NS dispersion at 10 ◦ C (B1) was most conducive
to the dispersion of NS in the cement paste, leading to the best cement paste properties.

4. Conclusions
The particle-size distribution of NS in the cement solution, distribution of ultrasonic dispersion energy, hydration heat, mechanical
strength, and the content of hydrate products was analyzed to study the influence of temperature on the dispersion of NS, and its effect
on the properties of cementitious materials was analyzed in this study. The following conclusions were drawn:

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Fig. 9. DTG thermograms of the cement hydration products at different curing ages. (a) 3 d and (b) 28 d.
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Fig. 10. Ca/Si atom ratios of samples with NS at different temperatures (a) 3 d and (b) 28 d.

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Fig. 11. Microstructures of cement pastes with NS at different temperatures at 3 d curing. (a) B1, (b) B2, (c) B3, and (d) B4.

(1) Ultrasonication could effectively disperse agglomerates in the NS solution, and the particle size of NS decreased with increased
ultrasonic power. From the relationship between the ultrasonic energy output, dispersion temperature, and particle-size dis­
tribution, there was no proportional relationship between the ultrasonic energy output distribution.
(2) A higher dispersion temperature can result in smaller NS particles but easier agglomeration in the cement solution. The addition
of NS could advance the induction period of cement and obtain a higher main hydration exothermic peak. The trend becomes
more significant with decreased dispersion temperature.
(3) The low-temperature dispersion of NS improved the properties of cement-based materials. The filling effect and high pozzolanic
activity of the NS dispersion at low temperatures can be effective when NS is fully mixed with cement and the consumption of
CH in the C–S–H gel is accelerated. NS dispersion helps obtain better mechanical strength and other properties in cement-based
materials, which may be related to the contribution of calcium silicate hydrate with low Ca/Si ratio formed by the reaction of
nano-silica and calcium hydroxide. SEM analysis showed that the degree of NS dispersion in the cement-hardened matrix was
the best when the dispersion temperature was 10 ◦ C. At this temperature, properties such as compressive strength were also the
most beneficial.

Credit author statement

Haibao Liu:Investigation,writing-Original draft preparation. Qiuyi Li:Experiment and investigation. Songyuan Ni: Investigation
and validation. Liang Wang: Supervision and Reviewing. Gongbing Yue: Investigation and validation. Yuanxin Guo: Reviewing and
Editing.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to
influence the work reported in this paper.

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Fig. 12. Microstructures of cement pastes with NS at different temperatures at 28 d curing. (a) B1, (b) B2, (c) B3, and (d) B4.

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