Construction and Building Materials 264 (2020) 120237

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Construction and Building Materials

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Review

Effect of carbon nanotubes on compressive, flexural and tensile strengths

of Portland cement-based materials: A systematic literature review
Laura Silvestro ⇑, Philippe Jean Paul Gleize
Laboratory of Application of Nanotechnology in Civil Construction (LabNANOTEC), Department of Civil Engineering, Federal University of Santa Catarina (UFSC), Brazil

h i g h l i g h t s

 Systematic literature review on the use of CNTs in cement-based materials.

 Characteristics of the CNTs used in the current research.
 CNT dispersion methods.
 Influence of CNTs on compressive, flexural and tensile strengths of cement-based materials.

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

Article history: Carbon nanotubes (CNTs) are materials with excellent properties. However, when incorporated into
Received 25 April 2020 cement-based materials, improvements in mechanical properties cannot always be guaranteed owing
Received in revised form 22 June 2020 to their difficult dispersion and low interfacial interaction with the matrix. A systematic literature review
Accepted 8 July 2020
was conducted to elucidate the influence of CNTs on compressive, flexural and tensile strengths of
cement-based materials. The incorporation of CNTs increased compressive strength by up to 30% and
flexural and tensile strengths by up to 50%. Furthermore, the optimal CNT content to achieve these
Keywords:
improvements is up to 0.1% by weight of cement (BWOC).
Carbon nanotubes
Cement-based materials
Ó 2020 Elsevier Ltd. All rights reserved.
Compressive strength
Flexural strength
Tensile strength

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2. Systematic literature review . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
3. Results and discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.1. Characteristics of carbon nanotubes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
3.2. Characteristics of the cementitious matrices. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.3. Dispersion methods. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
3.4. Mechanical properties. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.4.1. Compressive strength . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6
3.4.2. Flexural strength. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 7
3.4.3. Tensile strength . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 10
4. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
Declaration of Competing Interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
Appendix A. Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 11

⇑ Corresponding author.
E-mail address: laura.silvestro@posgrad.ufsc.br (L. Silvestro).

https://doi.org/10.1016/j.conbuildmat.2020.120237
0950-0618/Ó 2020 Elsevier Ltd. All rights reserved.
2 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
1. Introduction
CNTs are being used and researched in several fields owing to
their excellent thermal, electrical, and mechanical properties [1–
3]. These nanomaterials are tube-shaped structures constructed
from one-atom-thick rolled carbon sheets [4]. The chemical bond-
ing of carbon atoms is composed entirely of sp2 bonds, similar to
those of graphite, which gives CNTs high Young’s modulus and
high strength [4]. CNTs are classified as single-walled carbon nan-
otubes (SWCNTs) and multi-walled carbon nanotubes (MWCNTs)
based on the number of concentric tubes. Among the characteris-
tics of these materials, the tensile strength ranges between 50
and 500 GPa for SWCNTs and 10–60 GPa for MWCNTs [5]. The elas-
tic modulus values are 1 TPa and 0.3–1.0 TPa for SWCNTs and
MWCNTs, respectively [5,6]. According to Ma et al. [7], these prop-
erties make CNTs one of the most resistant and rigid materials.
In the civil engineering field, the application of CNTs in Portland
cement matrices has a high potential for increasing the mechanical
properties and durability of this type of composites, as CNTs can
improve the microstructure of cementitious materials and act as
reinforcement against the propagation of microcracks [8–12].
Although CNTs have excellent properties, when incorporated in
cementitious composites, they do not always guarantee good per-
formance because of two main limitations: 1) the difficulty of dis-
persing these nanomaterials, mainly because of their hydrophobic
nature and the strong van der Waals forces between them [13] and
2) a weak interfacial interaction between the nanomaterial and the
matrix [14].
Therefore, the results regarding the mechanical properties of
cementitious composites with the incorporation of CNTs are diver-
gent, as reported by several researchers [15–17]. Konsta-Gdoutos
et al. [16] noted that, while some studies show unrealistic
increases in mechanical properties, others report insignificant con-
tributions and, in some cases, even reductions in these properties.
Mohsen et al. [15] attributed these divergent results to the diffi-
Fig. 1. Stages of systematic literature review.
culty of dispersing these nanomaterials homogeneously in the
cement matrix.
To elucidate the influence of the incorporation of CNTs in
cementitious composites, mainly on compressive, flexural and ten-
sile strengths, this research aimed to perform a systematic litera-
ture review to map the main publications in recent years on the
incorporation of CNTs in Portland-cement materials. In addition,
the aim was to identify the main characteristics of the CNTs used,
the dispersion methods employed, and the information related to
the constitution of the cementitious matrices evaluated.
2. Systematic literature review
The systematic literature review consists of a scientific research
method with a rigorous and well-defined process to identify, select,
collect data, carefully evaluate, and describe the relevant contribu-
tions related to the subject under study [18]. Windle [19] men-
tioned that this type of review allows us to organize information
objectively and to identify knowledge gaps. In addition, it helps to
identify the main authors of the topic in question and to define
the research problem when it has not yet been formulated [20].
In this research, the method proposed by Ferenhof and Fernan-
des [20] was adopted for conducting a systematic literature review.
The method itself, called systematic search flow (SSF), consists of
four main steps: definition of the search protocol (which involves
defining the search parameters, searching databases, and manag-
ing the documents found), analysis, synthesis, and a writing stage.
Fig. 1 shows the details of the implementation of the four
method steps for the research in question, which is related to the
identification of the influence of the incorporation of CNTs on the
mechanical properties of Portland cement matrices. The defined
keywords were searched in the titles, keywords, and abstracts of
the articles and the search was carried out on April 22, 2019. The
search was restricted to articles published between 2014 and
 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237 3

2019 to include the most recent research in the field, thus identi- number, 97% of the works used MWCNTs because, compared to
fying the main trends followed. Furthermore, the main variables SWCNTs, they have a lower cost and a lower tendency to agglom-
that influence the compressive, flexural and tensile strengths of erate, which facilitates obtaining a more homogeneous dispersion
CNT-cementitious composites were collected from the articles [21].
included in the systematic review. Thus, the following information Approximately 75% of the studies applied non-functionalized
was collected: type, diameter, length, aspect ratio, apparent den- nanotubes, 18% used carboxyl group (–COOH) functionalized nan-
sity, specific surface area and functionalization type of CNT; CNT otubes, 5% used hydroxyl group (–OH) functionalized nanotubes,
dispersion method; ultrasonication parameters adopted; surfac- and 2% did not report the type of CNTs used. The most common
tant type and content used; cement matrix mix proportion; and procedure for grafting –COOH and –OH groups onto the surface
compressive, flexural and tensile strength values. of the nanotubes consists of treatment with a mixture of sulfuric
As shown in Fig. 1, the literature review on the incorporation of and nitric acid [22,23]. In this context, there are divergences
CNTs into cementitious matrices, considering the boundary condi- regarding the influence of nanotube functionalization with the
tions defined in Step 1, resulted in the download of 195 articles. groups previously mentioned on the mechanical properties of
The articles that did not evaluate the influence of incorporating cementitious composites. While some authors reported a good dis-
CNTs on the compressive, flexural or tensile strengths of cementi- persion and interface with the matrix [8,22], Isfahani, Li, and
tious composites, review articles, and numerical modeling were Redaelli [24] did not find significant differences in the compressive
excluded from this total, resulting in 99 articles that were selected and flexural strengths of composites with functionalized nan-
for the next reading stage. These articles are listed in the Supple- otubes with the –COOH group compared to the non-
mentary Material of this article. The main research information, functionalized ones.
as well as aspects related to the influence of the incorporation of Ahmed et al. [25] observed lower increases in the mechanical
CNTs on the main mechanical properties of cementitious compos- properties of cementitious composites with functionalized CNTs
ites, will be presented below. with –COOH and –OH groups compared to the composites with
non-functionalized CNTs. This behavior can be attributed to the
greater hydrophilicity of the functionalized nanotubes, which pro-
3. Results and discussion
motes greater absorption of the water available in the system, hin-
dering the cement hydration reactions [22]. Based on X-ray
Initially, a survey of the main characteristics of the articles
diffraction (XRD) findings, Ahmed et al. [25] observed that pastes
found in the literature review is presented. This survey helped to
with –COOH and –OH functionalized nanotubes presented a higher
identify the main authors related to the topic and will serve as a
amount of ettringite. These authors mentioned that ettringite dis-
basis for the definition of several variables of experimental pro-
turbs the densification of the calcium-silicate-hydrate (C-S-H) dur-
grams for future research, such as the w/c ratio of the cement
ing hydration, eventually producing voids that may prevent the
matrix, CNT content by weight of cement (BWOC), aspect ratio
pastes from reaching their mechanical performance potential.
and treatment type of CNT, dispersant type and content, among
Reales and Toledo Filho [26] also mentioned that some studies
others. In addition, the results of the compressive, flexural and ten-
have identified negative effects from the insertion of the functional
sile strengths reported in the articles included in the literature
groups –OH and –COOH on the surface of the CNTs, which can be
review are also presented, especially regarding the increase/de-
attributed to the tendency of these nanomaterials to agglomerate
crease percentage in relation to the CNT content.
owing to the negative surface charge associated with these func-
tional groups. This is because there is an interaction between the
3.1. Characteristics of carbon nanotubes CNTs and Ca(OH)2 that affects the stability of dispersions and gen-
erates an agglomeration phenomenon, hindering the electrostatic
Table 1 shows the main characteristics of the CNTs used in the repulsion between the negative functional groups on the surface
articles included in the systematic review. Regarding the total of the CNTs and the superplasticizer molecules that maintain the
CNTs dispersed [27].
Table 1
Characteristics of the carbon nanotubes described in the articles of Regarding the dimensions of the CNTs used, various articles
the systematic literature review. used nanotubes with average diameters of up to 30 nm. The most
frequent interval was between 10 and 20 nm, representing 28.2%
Type Number of articles
of the total works. The same trend was observed regarding the
MWCNT 96
average length; various articles used lengths reaching 30 mm, with
SWCNT 3
Functionalization Number of articles the 10–20 mm interval being the most significant, accounting for
Non-functionalized 74 36.4% of all works.
Functionalized (–COOH) 18 Mohsen et al. [28] evaluated the effect of MWCNT geometry on
Functionalized (–OH) 5 the dispersion, compressive, and flexural strengths of Portland
Not informed 2
Diameter (nm) Number of articles
cement pastes. CNTs with diameters of 10–20, 20–30, and 30–
<10 15 50 nm and lengths between 0.5 and 2 and 10–30 mm were evalu-
10 and <20 28 ated. The authors found that for CNT contents of up to 0.15% by
20 and <30 12 weight of cement (BWOC), CNTs with smaller diameters and
30 and <40 17
greater lengths resulted in the highest strength value. For CNT con-
40 and <50 3
50 17 tents of up to 0.25% BWOC, those with shorter lengths achieved
Not informed 7 greater strengths compared to the longer CNTs. In addition, the
Length (mm) Number of articles authors also noted that short CNTs (0.5–2 mm) had better disper-
<10 19 sion properties than those measuring 10–30 mm. The results
10 and <20 36
20 and <30 19
obtained by these authors are in agreement with Konsta-
30 and <40 6 Gdoutos, Metaxa, and Shah [29]. These authors evaluated the effect
40 and <50 1 of two types of MWCNTs measuring 10–30 mm (short) and 10–
 50 4 100 mm (long) on the mechanical properties of Portland cement
Not informed 14
pastes. Compared to short CNTs, long CNTs achieve the same level
4 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
of mechanical performance at lower concentrations. However, the
authors found that longer CNTs are more difficult to disperse.
3.2. Characteristics of the cementitious matrices
Table 2 shows the characteristics of the cementitious matrices
belonging to the 99 articles included in the systematic literature
review. Most studies evaluated the incorporation of CNTs in Port-
land cement pastes and mortars. Only 13% of the studies evaluated
this incorporation in concrete. Gillani et al. [30] noted that the
number of studies fully describing the use of CNTs in a concrete
matrix is limited, which may be related to the high cost of this
nanomaterial in relation to the other constituents of the concrete
matrix and the difficulty of dispersing large amounts of CNTs.
Furthermore, Hawreen, Bogas and Kurda [31] mention that the
main difference of concretes is the size of the aggregates, in which
larger aggregates will affect the CNT dispersion in the cementitious
matrix and the failure mode. The authors also highlight that in the
cases where the compressive strength is influenced by the inter-
face transition zone (ITZ) or by the aggregate strength, the cement
matrix quality assumes less relevance on the concrete strength,
what may justify the higher CNT reinforcement efficiency in
cement pastes and mortars than in concrete [31]. In this context,
Hawreen and Bogas [32] added that in conventional concrete,
beyond the cement matrix, the aggregate–matrix interface also
affects the mechanical performance, therefore, the modest
strength improvements in concretes may also be attributed to
the CNTs inability to significantly enhance the quality of the aggre-
gate–matrix bond.
Regarding the w/c ratio, approximately 40% of the articles eval-
uated the incorporation of CNTs in cementitious matrices with w/c
ratios within the range of 0.4 to 0.5 (Table 2). Therefore, Choi et al.
[33] analyzed the incorporation of 1.0% BWOC of MWCNTs and w/c
ratios of 0.40, 0.50 and 0.60 in Portland cement mortars. The com-
pressive strengths of these mortars at 7, 14 and 28 days are shown
in Fig. 2.
As can be seen in Fig. 2, for all ages the strength enhancement
for the MWCNT mortar with w/c ratio of 0.4 is higher than for
the MWCNT mortars with w/c ratio of 0.5 and 0.6. After 28 days
of curing, the compressive strength of the MWCNT mortar was
34%, 8%, and 4% greater than that of the OPC mortar when the w/
c ratio was 0.4, 0.5, and 0.6, respectively. Choi et al. [33] justify that
in systems with larger amounts of water, the reduction in com-
pressive strength with the incorporation of CNTs occurs because
these materials hinder the hydration reactions of Portland cement
during the initial curing phases, inducing weak bonds between the
hydration products. Besides that, in MWCNT mortar with lower
water content, the MWCNTs had a bridging effect on voids in the
hydration material, thereby increasing coherence inside the
cement mortar [33].
Hawreen et al. [17] also observed that the incorporation of CNTs
is more effective in mortars with low w/c ratios. The authors eval-
Table 2
Characteristics of the cementitious matrices of the articles
included in the systematic literature review.
Cementitious matrices Number of articles
Paste 39
Mortar 47
Concrete 13
w/c ratio Number of articles
0,2 and < 0,3 8
0,3 and < 0,4 22
0,4 and < 0,5 40
0,5 21
Not informed 8
Fig. 2. Compressive strengths at 7, 14 and 28 days of mortars with 1.0% by weight
of cement (BWOC) of CNT and reference mortars with different w/c ratios Choi et al.
[33].
uated the flexural strengths of mortars at 28 days with a 0.1%
BWOC of CNT and w/c ratios of 0.35, 0.45, 0.50, and 0.55. Compared
to their respective references, these mortars with added CNTs
showed increases in their flexural forces of 27%, 19%, 19%, and
21%, respectively. The authors attributed these results to the incor-
poration of superplasticizers in low w/c ratio mortars, contributing
to the dispersion of CNTs. In addition, they mentioned that more
CNTs are incorporated into low w/c ratio mortars because the
amount of CNTs is determined by the weight of the cement. Haw-
reen, Bogas and Kurda [31] observed the same trend previously
mentioned in relation to the influence of the w/c ratio on the effi-
ciency of CNT on the compressive strength of concretes.
However, Manzurand Yazdani [22] observed a different trend
from that reported by Choi et al. [33], Hawreen et al. [17] and Haw-
reen, Bogas and Kurda [31] regarding the influence of the w/c ratio
in cementitious matrices with the incorporation of CNTs. They
evaluated the compressive strengths of mortars with 0.3% BWOC
of MWCNTs and w/c ratios of 0.50, 0.55, 0.60, 0.62, 0.65, and
0.70. The system with a w/c ratio of 0.5 presented the worst
mechanical performance on days 7 and 28. A higher compressive
strength was observed in the mortar with a w/c ratio of 0.62, with
increments of 17.5% and 10.3% compared to the reference samples,
on days 7 and 28, respectively. To justify this behavior, the authors
mentioned that in systems with low w/c ratios, if CNTs are not well
dispersed, water can be trapped in CNT clusters; thus, hindering
hydration reactions and the formation of products that are essen-
tial for the development of matrix strength. The authors also added
that, in composites with higher w/c ratios, the solutions have a
higher amount of water and provide more space for the dispersion
of the CNTs, contributing to a uniform distribution of the CNTs in
the matrix.
3.3. Dispersion methods
Table 3 shows the number of articles included in the systematic
literature review related to the CNT dispersion methods. The most
widely used dispersion method consists of combining ultrasonica-
tion with a dispersant. These two approaches are used in combina-
tion because, while ultrasonication promotes a temporary
dispersion of the CNTs because of the permanent existence of
van der Waals forces, dispersants work by preventing agglomera-
tion and ensuring solution stability [4]. Of the 99 articles analyzed,
approximately 84% used ultrasonication and 77% used dispersants
 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
Table 3
CNT dispersion methods used in the articles of the systematic
literature review.
Dispersion methods Number of articles
Ultrasonication 83
Standard mixer 8 the interfacial tensions between the nanomaterials and the water.
Magnetic stirring 1 The physical adsorption of the surfactant on the surface of the CNT
Others 3
Not informed 4
Dispersant Number of articles
Yes 76
No 22
Not informed 1
Type of dispersant Number of articles
Polycarboxylate 40
Naphthalene 5 in Fig. 3. As can be seen in Fig. 3a, characterized by a surfactant
Others 23
Not informed 8 the amount of surfactant is insufficient to uniformly coat the entire
for the dispersion process. The most widely used dispersant was a
polycarboxylate-based additive, identified in 40.4% of the works.
Polycarboxylate-based admixtures contribute to the dispersion of
CNTs and the workability of cement mixes. Beyond
polycarboxylate-based and naphthalene-based dispersants, has
also been identified the use as dispersing agents of sodium dodecyl
sulfate (SDS), sodium dodecyl benzene sulfonate (SDBS), polyvinyl
pyrrolidone (PVP), among others, as can be seen in the Supplemen-
tary Material. Furthermore, 16 articles used only ultrasonication
without a dispersant.
As can be seen in the Supplementary Material of this research,
the lack of information in the reviewed articles on the ultrasonica-
tion parameters adopted, such as power, frequency, duration,
amplitude, and applied energy, makes it difficult to reproduce
the analyses and compare the results.
Ultrasonication involves the application of ultrasound energy to
disperse particles in a solution. The principle of this technique
involves the transfer of waves to form a cavitation field in which
the pressure differences causes the implosion of millions of
microbubbles. The accumulated energy of these microbubbles is
then released, promoting the exfoliation of the CNT clusters [4].
Regarding the parameters adopted for the dispersion of CNTs by
means of ultrasonication, Jarolim et al. [34] emphasized that atten-
tion is needed in relation to the energy supplied to the system. This
is because high energies can damage or even break CNT graphene
sheets, compromising the positive influence of these nanomateri-
als on the mechanical properties of cementitious composites.
Alrekabi et al. [35] mentioned that a high intensity (amplitude)
in combination with a short duration in the ultrasonication process
significantly improves the dispersion of CNTs and, consequently,
the mechanical properties of cementitious matrices with added
nanomaterials.
The use of dispersants for the dispersion of CNTs consists of a
non-covalent functionalization technique that has the main advan-
tage of not modifying the original characteristics of CNTs. Accord-
ing to Sahoo et al. [36], the non-covalent functionalization of CNTs
is of particular interest because it does not compromise the prop-
erties of such nanomaterials and improves their solubility. Baner-
jee, Hemraj-Benny, and Wong [37] noted that one of the main
advantages of this type of functionalization lies in the conservation
of the electronic structures of the CNTs, preventing the disturbance
of the intrinsic sp2 structures of the CNTs. However, its main disad-
vantage is the weak link formed between the CNT and the mole-
cule used, generating a low efficiency in the straining transfer at
the interface between such nanomaterials and the cementitious
matrix.
This type of functionalization mainly involves the use of surfac-
tants and coating with polymers. According to Van Herk [38], sur-
5
factants are amphiphilic molecules composed of hydrophilic and
hydrophobic segments. Surfactant molecules act on the surface of
CNTs and normally direct the hydrophobic group towards the sur-
face of the CNTs and expose the hydrophilic group to the water.
This makes the surface of CNTs hydrophilic and, as a result, reduces
reduces the surface tension of the nanomaterial and, owing to elec-
trostatic/steric repulsion mechanisms, overcomes the existing van
der Waals attraction forces; thus, preventing the formation of
agglomerates and contributing to nanomaterial dispersion [7].
The adsorption mechanism of the surfactant molecules on the
surface of the CNTs as a function of their concentration is shown
concentration below the critical micellar concentration (CMC),
CNT surface, being ineffective in preventing the agglomeration of
CNTs and ensuring good dispersion of these nanomaterials. When
the critical micellar concentration is reached, the CNT surface is
completely covered by the surfactant molecules (Fig. 3b). Surfac-
tant concentrations higher than the CMC do not promote an
increase in the dispersion of CNTs and cause the formation of
micelles (Fig. 3c) [2].
According to Van Herk [38], micelles are aggregates of surfac-
tant molecules, usually spherical, with dimensions of a few
nanometers. Jiang, Gao, and Sun [39] mentioned that the osmotic
pressures of the micelles in classic colloidal suspensions and CNT
dispersions create an attraction effect called depletion. Thus, these
authors mentioned that the surfactant concentration must be close
to the CMC because, in dispersions with concentrations below the
CMC, van der Waals forces cause CNT agglomeration; additionally,
at high surfactant concentrations (above CMC), there is a tendency
for these nanomaterials to agglomerate because of the depletion
effect mentioned above. In addition, it is important to consider that
the use of high levels of surfactants for the dispersion of CNTs can
impair the mechanical performance of Portland cement matrices
owing to the air-incorporating characteristic of such molecules
[40].
Collins, Lambert, and Duan [41] evaluated the performance of
eight types of dispersants on CNT dispersions in aqueous solution
based on a visual analysis of the sedimentation of the solutions
over time. The solutions composed of CNTs, dispersants, and water
were initially subjected to magnetic stirring and then to ultrason-
ication for 12 min. The eight types of dispersants analyzed by the
authors were air-entraining based on sodium alkylbenzene sul-
fonate (AEA), styrene-butadiene rubber copolymer (SBR), propy-
lene glycol aliphatic ether (SR), two types of polycarboxylates,
calcium naphthalene sulfonate (CNS), derived from naphthalene
sulfonic acid (NSAD), and lignosulfonate (WDRA). The results indi-
cated that the polycarboxylates promoted better dispersion and
stability of the CNT solutions in an aqueous medium, as well as
better performance in relation to the mechanical properties of
cementitious composites with the addition of CNTs. For a w/c ratio
of 0.35, the compressive strengths at 28 days of Portland cement
pastes composed of nanotubes and polycarboxylate-based admix-
tures were approximately 25% higher than the reference paste, cor-
roborating the existence of a good dispersion of the nanomaterial
in question when such admixtures are used.
Kim et al. [42] used three types of superplasticizers as CNT dis-
persing agents, evaluating the characteristics of CNT dispersions in
aqueous solution using UV–Vis spectroscopy and zeta potential.
They also analyzed the dispersion of CNTs in cementitious matrices
through electrical resistivity. The three types of superplasticizers
had the following compositions: Type A (lignosulfonate + polycar
boxylate), Type B (naphthalene + lignosulfonate), and Type C (poly-
carboxylate). The solutions were composed of water, CNTs, and a
6 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
Fig. 3. Schematic representation of the adsorption of surfactant molecules on the CNT surface: a) surfactant concentration below the critical micellar concentration (CMC); b)
surfactant concentration equal to CMC; c) surfactant concentration above the CMC (showing micelle formation). Sobolkina et al. [2].
superplasticizer and were dispersed by ultrasonication. Although
the results obtained by UV–Vis spectroscopy and zeta potential
tests indicated a better dispersion and stability of the solution with
the Type B superplasticizer, the electrical resistivity results of the
cement-CNT composites at 28 days indicated that the composites
made up of the type A and C superplasticizers showed lower elec-
trical resistivity. Therefore, it can be inferred that superplasticizers
A and C contributed to a better dispersion of CNTs owing to the for-
mation of a homogeneous network for the conduction of electricity
in these composites. Hence, the authors concluded that polycar-
boxylate superplasticizers are effective in dispersing CNTs in
cementitious composites.
Cui et al. [43] performed a comparative study on the dispersion
of MWCNT-OH in water with four types of dispersants, i.e.,
polyoxyethylene-alkyl phenol ether (APEO), silane-modified poly-
carboxylate (Silane-PCE), and two types of cationic polycarboxy-
lates (IC-PCE and II-C-PCE). To compare the dispersion capacity
of these four dispersants and to establish an optimal CNT/disper-
sant ratio, dispersions composed of 1 g/L CNT and dispersant con-
centrations between 0.1 and 14 g/L were prepared using
ultrasonication with an amplitude of 30% and a duration of
30 min. The results obtained by UV–Vis spectroscopy indicated
that the dispersion capacity of the four dispersants followed the
next order: APEO > I-C-PCE > Silane-PCE > II-C-PCE. In addition,
the optimal dispersant/CNT ratio (identified by the maximum
absorbance value of 600 nm) was 1:5, 2:1, 4:1, and 12:1 for APEO,
IC-PCE, II-C-PCE, and Silane-PCE dispersants, respectively. The
improved performance of the APEO dispersant can be attributed
to the presence of the benzene ring in its structure, which pro-
motes greater adsorption on the surface of the CNTs. The greater
dispersion capacity of the IC-PCE dispersant is associated with a
shorter hydrophilic chain than that of II-C-PCE, as this characteris-
tic reduces the possibility of the occurrence of micelles and, conse-
quently, the depletion effect that can generate agglomeration of
CNTs in aqueous solutions [43].
Liebscher et al. [44] noted that the dual functionality of
polycarboxylate-based superplasticizers, regarding the dispersion
of CNTs and the workability of cementitious composites, prevents
the insertion of another dispersant in the mixture that may cause
adverse reactions in Portland cement matrices. Therefore, the
authors evaluated the influence of the main chain length and the
side chain length and density of the superplasticizer molecules
on the dispersion capacity of CNTs in aqueous suspensions. Addi-
tionally, they synthesized eight types of polycarboxylate-based
superplasticizers by varying the parameters mentioned above
and evaluated the degree of dispersion qualitatively through opti-
cal microscopy. The results indicated that the most efficient poly-
carboxylate for dispersing CNTs was characterized by a long
main chain and a high-density side chain. As for the side chain
length, there was no significant effect on dispersibility by such
admixtures [44].
Furthermore, Liew, Kai, and Zheng [4] mentioned that disper-
sants that are not beneficial for cement particle hydration should
be avoided. Thus, for the dispersion of CNTs, the authors recom-
mended the use of superplasticizers or dispersants with a similar
structure.
3.4. Mechanical properties
3.4.1. Compressive strength
One of the main objectives of this systematic literature review
was to elucidate the influence of the incorporation of CNTs on
the compressive strength of cementitious matrices. Thus, Fig. 4
presents a survey of the increase/decrease percentages of the com-
pressive strengths of cement-based materials with CNTs at 28 days
derived from the literature review. Of the 99 articles included in
the review, 91 showed results for compressive strengths at 28 days.
Of this total, approximately 94% of the articles reported increases
in compressive strengths with the incorporation of CNTs, while
only 6% of these articles reported lower resistances compared to
the reference matrix. Notably, only the configurations with the
best performances were considered in this study, i.e., the carbon
nanotube contents that promoted the greatest increases in relation
to the reference matrix. Likewise, in cases where the performance
was negative, the configurations that generated the least reduc-
tions in compressive strength were considered.
After analyzing Fig. 4, it was identified that only 6 articles
reported decreases in compressive strength with the incorporation
of CNTs [40,45–49]. According to Mendoza-Reales, Sierra-Gallego,
and Tobón (2016) [45] and Zhou et al. [47], the reductions in com-
pressive strength observed can be attributed to the agglomeration
of CNTs.
The negative performance observed by Hongyu et al. [40] can be
associated with the high percentage of CNTs and the dispersion
process used, as a 1.5% CNT content based on cement weight was
used; moreover, the nanomaterial was added directly to the
 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
Fig. 4. Percentages of increase/decrease in compressive strength at 28 days of age of cement-based materials with CNTs reported in the 91 articles found in the systematic
literature review.
cement and dry-mixed for only 5 min, without using a dispersant.
Even in the other configurations evaluated by these authors, corre-
sponding to pastes composed of 1.5% BWOC of CNTs and three dif-
ferent types of dispersants (sodium dodecyl sulfonate (SDS),
Tween-20, and Triton X-100) subjected to ultrasonication for the
dispersion of nanomaterials in water prior to addition to cement,
the authors found even more pronounced reductions in compres-
sive strength compared to the system in which dry dispersion of
CNTs was used. According to Hongyu et al. [40], this may be a con-
sequence of air incorporation caused by the dispersants used. Kim
et al. [46] used 0.5% BWOC of CNT and a dry mixing procedure for
cement and CNTs mixing without ultrasonication, which may jus-
tify the decrease in compressive strength compared to the refer-
ence Portland cement paste.
Szelag [48] produced Portland cement pastes with a content of
0.1% BWOC of CNT, using ultrasonication for dispersion together
with an SDS-based surfactant. According to Szelag [48], the reduc-
tion in compressive strength of the pastes with the addition of
CNTs is a function of the incorporation of air by the surfactant,
resulting in an increased porosity of the cementitious matrix.
According to Wang et al. [49], the reduction in compressive
strength observed may be related to the poor dispersion of CNT-
OH (0.5% BWOC) in concretes, which, unlike mortars, have coarse
aggregates in their composition. Therefore, the authors mentioned
that the effect of adding CNTs in concrete is not yet consistent and
requires further studies.
As shown in Fig. 4, 74% of the 91 articles analyzed reported
increases in compressive strength of up to 30% after 28 days, with
numerous works in the 10–20% increase range. In approximately
19% of the studies, increments equal to or higher than 30% were
found. Reales and Toledo Filho [26] mentioned that the increases
in compressive strength caused by the incorporation of CNTs can
generally be explained by the nucleation effect. The decreases are
attributed to the competition between the CNTs and the cement
particles for the superplasticizers, agglomeration of the CNTs,
adsorption of the mixing water by the hydrophilic groups present
on the surface of the CNTs, and the type of dispersant used, as it
can affect the cement hydration reactions.
According to Liew, Kai, and Zhang [4], there are four main
mechanisms in the reinforcement of cementitious matrices using
CNTs:
7
 CNTs can fill pores ranging from 10 to 103 nm with hydration
products. This effect promotes an efficient stress transfer
between the CNTs and the matrix, delaying the development
of cracks on a nanometer scale and hindering the formation of
micropores. Xu, Liu, and Li [9] found that the addition of
MWCNTs to Portland cement pastes reduces porosity and total
pore volume of the matrix. Furthermore, there was a trend
towards a reduction in pore size with an increase in CNT con-
tent, as well as a significant reduction in pores larger than
50 nm.
 CNTs reduce the nanoporosity of the cementitious matrix by
filling the spaces between the hydrate gel.
 CNTs can modify the microstructure of hydration products.
Singh et al. [50] detected through XRD that new components
were created because of the chemical bonds between the CNTs
and hydrates in the cementitious matrix. Furthermore, Barb-
huiya, and Chow [51] observed through a nanoindentation test
that the addition of CNTs increased the amount of high-density
C-S-H particles.
 CNTs can act as nucleating agents for the C-S-H gel.
Another aspect to be considered in relation to the effect of CNTs
on the mechanical properties of Portland cement matrices is the
CNT content used, as there is a tendency for this nanomaterial to
agglomerate beyond an optimal percentage. In this case, as previ-
ously mentioned, the CNT contents that promoted the highest
increases in compressive strength at 28 days were selected. Fig. 5
shows the CNT addition content as a function of the increases/de-
creases in compressive strength reported in the 91 articles that
evaluated this mechanical property. There is a concentration of
points in the content addition of up to 0.1% BWOC CNT. In approx-
imately 50% of the total 91 studies, the optimal CNT content
observed was within this range. This finding corroborates the
information reported by Reales and Toledo Filho [26]. These
authors mentioned that the optimal CNT content is usually below
0.1% BWOC.
3.4.2. Flexural strength
Fig. 6 shows a survey of the percentages of increase/decrease in
flexural strength at 28 days of cement-based materials with CNTs
in the articles analyzed in this literature review. Of the 99 articles
8 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237

Fig. 5. CNT content as a function of the percentage of increase/decrease in compressive strength of cement-based materials with CNTs.

Fig. 6. Percentages of increase/decrease in flexural strength at 28 days of cement-based materials with CNTs reported in the 57 articles found in the systematic literature
review.

included in this review, 57 presented results of flexural strength at
28 days. From this total, approximately 92% of the articles reported
increases in flexural strength with the incorporation of CNTs, while
only 8% of them reported lower resistances compared to the refer-
ence matrix. It is important to note that in this survey, only the
configurations with the best performances were included, i.e.,
CNT contents that promoted the largest increments in relation to
the reference and, in cases where the performance was negative,
the configurations that generated the lowest decreases in flexural
strength.
As shown in Fig. 6, only four studies reported reductions in flex-
ural strength caused by the incorporation of CNTs in Portland
cement matrices [45,48,49,52]. Mendoza-Reales, Sierra-Gallego,
and Tobón [45] attributed this result to the tendency of CNT
agglomeration. Szelag [48] and Tragazikis et al. [52] attributed this
behavior to the higher porosity of the CNT pastes caused by the
incorporation of air resulting from the dispersants used, which in
the first case were SDS-based and in the second case were
polycarboxylate-based. Wang et al. [49] mentioned problems in
dispersing CNTs functionalized with hydroxyl groups.
However, evidence shows that CNTs are usually effective in
increasing the flexural strengths of cementitious matrices. Approx-
imately 74% of the works analyzed in this study reported an
increase of up to 50% in flexural strength (Fig. 6). Notably CNTs
have a greater impact on increasing the flexural strength of cement
matrices than on compressive strength. Konsta-Gdoutos et al. [13]
also observed higher improvements on the flexural strength and
flexural toughness of MWCNTs mortars in contrast to modest
 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237 9

improvements on the compressive strength, what can be attribu-
ted to a more controlled crack coalescence process at the nano
and microscale. This increased energy absorption capability sug-
gests that a significant amount of energy is required for the mate-
rial to fail and for the cracks to propagate [13]. In this context,
according to Sindu e Sasmal [53], CNTs acted only as fillers when
subjected to compression whereas under tension, it contributes
in bridging the cracks at nanoscale, thereby delaying the failure
of the material.
Sedaghatdoost and Behfarnia [54] evaluated the flexural
strengths of Portland cement mortars with the addition of
MWCNTs at percentages of 0%, 0.05%, 0.1%, and 0.15% BWOC. The
nanomaterial was dispersed by ultrasonication in combination
with a polycarboxylate-based superplasticizer. At 28 days, all con-
figurations with CNTs showed higher flexural strengths. The refer-
ence showed a flexural strength of 6.49 MPa and the mortars with
CNT percentages of 0.05%, 0.1%, and 0.15% BWOC showed values of
7.06 MPa, 7.22 MPa, and 6.81 MPa, respectively. According to
Sedaghatdoost and Behfarnia [54], the higher flexural strengths
of mortars with CNTs can be attributed to the physical contribution
of CNTs through the filling of the pores between the C-S-H and the
ettringite and the consequent reduction in the porosity of the
cementitious matrix. Moreover, Naeem et al. [55] also mentioned
that dispersed CNTs act by linking microcracks and by restricting
the propagation of cracks, improving the mechanical properties
of cementitious composites. Hawreen, Bogas, and Dias [17] incor-
porated 0.05% BWOC of functionalized CNTs with carboxyl and
hydroxyl groups in Portland cement mortars with a w/c ratio of
0.5, showing increases in flexural strength at 28 days of approxi-
mately 14.6% for both types of CNTs. To identify changes in the
mortar microstructure, the cementitious matrices were analyzed
using a scanning electron microscope. The micrographs obtained
by the authors are shown in Fig. 7. The CNTs were well dispersed
in the matrix and the crack bridging mechanism promoted by
these nanomaterials was observed.
According to Hawreen, Bogas, and Dias [17], in cracks with
small openings, CNTs can effectively transfer loads through these
spaces. However, it is important to note that this mechanism only

Fig. 7. Micrograph of Portland cement mortars with w/c ratios of 0.5 and 0.05% by weight of cement (BWOC) of CNT a) CNTs functionalized with –COOH groups and b) CNTs
functionalized with –OH groups (a single arrow indicates the CNT and the double arrow indicates the ettringite) Hawreen, Bogas, and Dias [17].

Fig. 8. Relationship between CNT content and percentage of increase/decrease in flexural strength of cement-based materials with CNTs.
10 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237

Fig. 9. Percentages of increase/decrease in tensile strength at 28 days of cement-based materials with CNTs reported in the 19 articles found in the systematic literature
review.

occurs in cracks with openings approximately 1 mm wide. In addi-
tion, the authors also observed higher amounts of ettringite in
mortars with CNTs functionalized with –COOH and –OH groups.
This occurs because treatment with acid can result in sulfate ions
to remain on the CNT surface. The ettringite crystals in matrices
with CNTs functionalized with –COOH and –OH groups explain
the lower increases in mechanical properties compared to those
of non-functionalized CNTs, as these crystals can cause localized
detachments and reductions in matrix strength.
Fig. 8 shows the relationship between CNT content and the per-
centage of increase/decrease in flexural strength reported in 57
articles that evaluated this mechanical property included in this
systematic literature review. In approximately 61.4% of the 57
studies, the optimal CNT content observed was up to 0.1% BWOC.
This trend was also observed for the compressive strength, indicat-
ing an optimal addition range concerning the mechanical proper-
ties of Portland cement composites with CNTs.
3.4.3. Tensile strength
Fig. 9 shows a survey of the percentages of increase/decrease in
tensile strength at 28 days of cement-based materials with CNTs in
the articles analyzed in this systematic literature review. Of the 99
articles included in this review, only 19 presented results of tensile
strength at 28 days. From this total, all articles reported a equiva-
lent performance or increases in tensile strength with the incorpo-
ration of CNTs. Furthermore, approximately 80% of the works
analyzed in this study reported an increase of up to 50% in tensile
strength. This is because the CNTs, due to their shape and high ten-

Fig 10. Relationship between CNT content and percentage of increase/decrease in tensile strength of cement-based materials with CNTs.
 L. Silvestro, P. Jean Paul Gleize / Construction and Building Materials 264 (2020) 120237
sile strength, could act like a bridge or fiber in the cement matrix,
being able of bond efficiently to the matrix and effectively bridging
the nanocracks [54].
Baloch, Khushnood and Khaliq [56] mention that the initiation,
propagation and coalescing of the induced cracks reduce the load
carrying area of any cementitious matrix and that this reduction
of effective load bearing area increases the tension at critical crack
tips. Thus, CNTs introduces additional closing that provides resis-
tance to the crak growth. Furthermore, it is important to consider
that crack coalescence under tensile loading causes more cracking
compared to compressive load, where some cracks tend to close-
up as well [56]. This may justify the greater contributions of CNT
in tensile strength compared to compressive strength.
Fig. 10 shows the relationship between CNT content and the
percentage of increase/decrease in tensile strength reported in 19
articles that evaluated this mechanical property included in this
systematic literature review. In approximately 68% of the 19 stud-
ies, the optimal CNT content observed was up to 0.1% BWOC. This
trend was also observed for the compressive and flexural strengths,
indicating an optimal addition range concerning the mechanical
properties of Portland cement composites with CNTs.
4. Conclusions
A systematic literature review on the incorporation of CNTs into
cementitious matrices covering 99 articles indicated that:
 MWCNTs were used in 97% of the studies.
 Approximately 75% of the studies used CNTs without function-
alization, 18% used CNTs functionalized with the carboxyl group
(–COOH), 5% used CNTs functionalized with the hydroxyl group
(–OH), and 2% of the works did not report the type of CNTs used.
Therefore, the importance of exploring different CNT functional-
ization techniques to improve the dispersion and interface with
the cement matrix is highlighted.
 Several studies have been carried out using CNTs with an aver-
age diameter of up to 30 nm and a length of up to 30 mm.
 Many studies have evaluated the incorporation of CNTs in Port-
land cement pastes and mortars; however, only 13% used
concrete.
 In approximately 40% of the studies included in this review, the
w/c ratios were between 0.4 and 0.5. As reported in the litera-
ture, w/c ratios close to 0.4 enhance the positive effect of CNTs
on the mechanical properties of cementitious matrices.
 Ultrasonication in combination with a polycarboxylate-based
dispersant was the most widely used dispersion method in
most studies. Concerning the ultrasonication parameters, high
intensity in combination with a short duration significantly
improves the dispersion of CNTs and, consequently, the
mechanical properties of the cementitious matrices with the
incorporation of these nanomaterials.
 The incorporation of CNTs increases compressive, flexural and
tensile strengths if they are properly dispersed. In the studies
included in this systematic review, increases in compressive
of up to 30% and in flexural and tensile strengths of up to 50%
were observed.
 The optimum CNT content for improving compressive, flexural
and tensile strengths is 0.1% BWOC.
Therefore, it is possible to conclude that these types of nanoma-
terials promote a positive effect on such properties if properly dis-
persed. In addition, considering the excellent properties of CNTs,
there seems to be a potential for further increasing the mechanical
properties of cement-based materials using this nanomaterial.
Research should focus on ways to improve both the dispersion of
11
CNTs and the interface with the matrix, as well as to minimize
the negative effect of air incorporation resulting from the use of
dispersants that aim to ensure the dispersion of nanomaterials.
This is important because, for the application of this nanomaterial
to be feasible for improving building materials, given its high cost,
it is essential to obtain significant increases in durability and desir-
able mechanical properties.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgments
The authors gratefully acknowledge the Brazilian government
research agencies – National Council for Scientific and Technolog-
ical Development (CNPq) and Santa Catarina Research Foundation
(FAPESC) – for providing financial support for this research, as well
as the National Institute on Advanced Eco-efficient Cement-based
Technologies (CEMtec) grant 465593/2014–3. Additionally, we
acknowledge the Coordination for the Improvement of Higher Edu-
cation Personnel (CAPES) for having granted a scholarship to the
first author.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.conbuildmat.2020.120237.
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