Carbon-Based Nanomaterials Engineered Cement Composites: A Review

Lu and Zhong J Infrastruct Preserv Resil (2022) 3:2 Journal of Infrastructure
https://doi.org/10.1186/s43065-021-00045-y
Preservation and Resilience
REVIEW Open Access
Carbon-based nanomaterials engineered

cement composites: a review
Dong Lu1,2 and Jing Zhong1,2*
Abstract
Carbon-based nanomaterials (CNMs) have been extensively used to modify cement matrix thanks to their extraordi-
nary specific surface area, high aspect ratio, and high strength and modulus. This review focuses on the current status
of research on CNMs modified cement composites, especially the progress made in the past decade (from 2011 to
2021). At first, the primary properties of typical CNMs used for manufacturing cement composites, the treatments
used to effectively disperse CNMs in water and cement matrix, and the corresponding characterization methods
are reviewed. And then, the effects of introducing CNMs on the properties of cement composites (both fresh and
hardened) are also discussed in this work. Finally, the knowledge gaps and remaining challenges for future work are
discussed.
Keywords: Cementitious composites, Carbon-based nanomaterials, Dispersion, Cement hydration, Rheology
properties, Reinforcing mechanisms
Introduction (SCMs) [13, 15], the application of some new cementi-

Cement concrete is the most widely used man-made tious binders [9, 16], and using nanomaterials to modify
material in modern civil engineering because of the low cement matrix [5, 17], etc. Among them, the ultra-fine
cost and long service time [1–3]. Typically, it is regarded particles-nanomaterials, show great potential to increase
as a type of material with high compressive strength and the density of microstructure and finally improve the
durability [4, 5], however, the inherently quasi-brittle mechanical and durability properties of cementitious
behavior (e.g., poor tensile strength and crack propaga- composites.
tion) has limited its structural applications [6–9]. Fur- Advancement in nanotechnology and nanomateri-
thermore, the cement or concrete industry is high energy als over the past decade has provided invaluable oppor-
consumption and has a substantial environmental foot- tunities to improve the microstructure of cementitious
print [3, 10]. It has been reported that the global cement composites at the nanoscale [5, 18]. Typically, the intro-
production was around 4.5 billion tons and the CO2 duction of nanomaterials at a very small dosage can result
emission was reached be approximately 1.45 Gt in 2019 in a significant improvement in the performance (e.g.,
[3, 11]. In 2020, the energy consumption of the cement mechanical, chemical resistance, and transport proper-
industry in China was estimated at approximately 349.4 ties, etc.) of cement-based materials [12, 19, 20], with
tons [10, 12]. These years, attempts have been adopted mechanisms of nano-filling [21, 22], nucleation effect [23,
to develop high-performance concrete or low-carbon 24], and pozzolanic reactivity (nano-SiO2) [25, 26], etc.
cementitious materials [12–14], such as partially replac- Carbon-based nanomaterials (CNMs), including carbon
ing cement with supplementary cementitious materials nanotubes (CNTs) [27, 28], carbon nanofibers (CNFs)
[29, 30], graphene [31], and graphene oxide (GO) [32],
*Correspondence: [email protected] are very promising candidates as additives in the cement
1
School of Civil Engineering, Harbin Institute of Technology, 73 Huanghe matrix [24, 31, 33–35], which are abundant in nature and
Road, Harbin, Heilongjiang 150090, P. R. China have already achieved industrialized mass production.
Full list of author information is available at the end of the article
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Lu and Zhong J Infrastruct Preserv Resil (2022) 3:2 Page 2 of 20
For instance, the annual production of typical CNTs in quantitatively assess the dispersion quality of CNMs in a
China is approximately 500,000 tons. Currently, the price cement matrix; And (ii) what types of CNMs have nucle-
of CNTs is in the range of 80-120 RMB/kg, depending ation effect and significantly affect cement hydration.
on the quality and number of walls, while the prices of In this context, the properties of CNMs used in cement
graphene and GO are expected to be in the range of 400- materials are introduced at first. Then the different dis-
450 RMB/kg and 350-400 RMB/kg in near future, respec- persion methods employed to manufacture cement
tively (http://www.nanotubes.com.cn.). Generally, the composites and the current evaluation methods are sum-
addition amount of CNTs, graphene, and GO (by weight marized. Next, we discuss the hydration and rheological
of cement) are 0.01-0.15 wt% [30], 0.01-2.5 wt% [36], properties of a fresh mixture for a better understanding
0.01-1.0 wt% [37], respectively. As such, it can be esti- of the influence of admixed CNMs in a cement hydration
mated that the addition of 0.01 wt% CNTs, graphene, and system. Finally, the influences of CNMs on the mechani-
GO could increase the cost per ton of cement in concrete cal and durability properties of hardened cement com-
production by approximately 8-12 RMB, 40-45 RMB, posites are reviewed.
and 35-40 RMB, respectively. According to the published
literature, the addition of 0.01 wt% GO can increase the Properties of CNMs and their morphology
28-d compressive strength of cement composites by In this review work, we only discussed one-dimensional
about 20-30% [37], thus, it can be estimated that the cost (1D) nanofibers (CNTs and CNFs) and two-dimensional
of cement reduces by approximately 130 RMB/ton for (2D) nanosheets (graphene and GO), the properties of
equivalent strength (the strength of GO/cement-42.5 has which are presented in Table 1 and Fig. 1, because they
roughly the same strength with cement-52.5), more than are the most studied CNMs in enhancing cement materi-
enough to cover the expense for GO addition. This could als during the last decade [19, 20, 50–54].
trigger a substantial economic benefit and alleviate the CNT (or CNTs) has a 1D concentric tubular structure
undesirable impacts of C O2 emission on the ecological with a hexagonal arrangement of carbon atoms and they
environment. were firstly reported by Iijima in 1991 [55]. The qual-
Unfortunately, although the application of CNMs ity, property, and production of CNTs were continu-
showed great potential in cement modification, their ously improving since then. The diameter and length of
broad application is still limited due to the poor disper- CNTs are typically in the range of 1-100 nm and 1-100
sion quality, as well as the controversial understanding μm, respectively, resulting in a very high aspect ratio
of the effects of CNMs on cement hydration [20, 24, 27]. and thus severe entanglement with each other [56–58].
Additionally, basic mechanisms for cement reinforce- These physical crosslinking, together with Van der Waal’s
ment of these CNMs are still under debate [20, 22, 24, 38, interaction between CNTs, making their dispersion very
39]. To this end, it is urgent to review the current knowl- challenging in water or cement matrix [28, 59]. It is well
edge related to the use of CNMs in cement composites known in the CNTs community that, for a given disper-
and accelerate their practical applications. It is believed sion method, the dispersion quality is highly dependent
that these gaps fundamentally stem from the failure to on the CNTs tortuosity and aspect ratio, both of which
thoroughly address the following questions: (i) how to largely determine the entanglement degrees [59, 60].
Table 1 The primary properties of CNMs used for preparing cement composites
Component CNTs CNFs Graphene GO
a
Diameter/thickness (nm) 0.4-2.0 (SWCNTs) 0.5-100 ~1 ~0.67
1.0-100 (MWCNTs)a
Aspect ratio 1000-10,000 100-1000 600-600,000 1500-45,000
SSAa (m2/g) 20-1315 100-1000 700-1500 2000-2600
Elastic modulus (GPa) >1000 6-200 >1100 >300
Tensile strength (GPa) 50-200 400-600 ~125 >112
Resistivity (Ω∙cm) ~10-2 0.1 - -
Thermal conductivity W/(m·K) ~6600 20-1950 - -
Special applications For structural health monitoring [28, 40–43]. Electromagnetic protection Accelerating cement
[31, 44, 45]. hydration [20, 24, 39,
46].
a
SWCNTs and MWCNTS are single-wall CNTs and multi-walled CNTs, respectively. SSA is a specific surface area
Fig. 1 The roles of the typical 1D nanofibers (CNTs and CNFs) and 2D nanosheets (graphene and GO) in cement composites [19, 22, 28, 34, 39, 45,
47–49]. G represents graphene
CNFs are cylindrical nanostructures with graphene lay- strength, high modulus, and outstanding electrical con-
ers arranged as stacked cones, which can be viewed as ductivity, are in-plane properties, essentially resulted
fiber-shaped nanomaterial with a length ranging from from the in-plane sp2 carbon-carbon bonds [63, 67].
50 nm to 200 nm [45, 61]. CNFs have similar geomet- Interestingly, because of the extremely small thickness
rics and physical properties with CNTs, yet with much of graphene, it can also be considered to be soft mat-
lower price (generally one-fifth of the price of CNTs), and ter. According to the previous reports, GO has a simi-
thus also extensively employed as an additive for cement lar bending stiffness with graphene (assuming a similar
matrix modification [30, 62]. Owing to the potential thickness), is in the order of 2 kT [63, 68, 69], meaning
micro (and nano) improvement of the interfacial tran- that these single-layer 2D materials can be easily buck-
sitional zone (ITZ), CNFs demonstrate a great potential led and a considerable amount of wrinkles will be natu-
to improve the mechanical strengths of cement materi- rally formed [63, 64, 66]. Such features could affect the
als [34]. Additionally, CNMs (especially graphene, CNTs, interaction between graphene (and its derivatives) with
and CNFs) demonstrate great potential to develop smart matrix materials [36, 59, 70, 71]. Because single-layer gra-
cement composites in the future. phene with atom thickness and perfect crystal structure,
Strictly speaking, graphene is a one-atom-thick flat which cannot be yielded at a large scale currently, the
nanosheet of s p2 bonded carbon atoms, it is arranged in commercially available materials claimed as “graphene”
a honeycomb-like lattice [63–65], which is the mother are actually multi-layers thin graphite [63, 64, 68]. They
of all graphitic materials, such as fullerenes, CNTs, and are mostly synthesized by exfoliation of graphite either
graphite [64, 66]. Note that, most of the excellent phys- by intercalation followed by mechanical shearing [63,
icochemical characteristics of graphene, such as excellent 64, 72]. According to classical plate theory, the bending
stiffness of plates is inversely proportional to the cubic degree of cement hydrates [20, 24], and regulate the
thickness [63–65]. Implying that the bending stiffness of formation of hydration crystals [46, 79, 80]. With these
multi-layer graphene with ~30 nm (corresponding to 100 advantages, GO has been the most studied CNMs for the
layers), which is six orders of magnitude higher than that modification of cement materials during the past decade
of the single-layer graphene [63, 64, 68, 72]. Such huge (as depicted in Fig. 3).
different bending stiffness could significantly change gra-
phene-cement interactions. Dispersion and characterization of CNMs in water
Another strategy to synthesize graphene is to chemi- and cement matrix
cally reduce GO [64, 73, 74], which can be readily Challenges for CNMs dispersing
obtained by oxidation of graphite in strong acid, as firstly As mentioned above, the possible agglomeration of
reported more than a century ago [64, 68, 72, 74]. Fig. 2 CNMs in the cement matrix are defects and negatively
illustrates the GO synthesis process. In short, the gap affect the properties of cement composites [19, 28, 53,
between adjacent layers in graphite greatly increased due 81–83]. That is, a high dispersion quality of CNMs is a
to the functionalization of graphene, mainly by carboxy- prerequisite for the effective reinforcement of cement-
late and epoxy groups, thus effectively decreased Van based materials [8, 44]. However, it is still very challeng-
der Waal’s interaction between graphene layers, allowing ing to realize an excellent dispersion of CNMs in the
easy exfoliation into single layers in water [64, 65]. There- cement matrix, since the strong Van der Waal’s attraction
fore, single-layer GO dispersion with high quality was between CNMs, as well as the complex electrolytic envi-
easy to prepare. More importantly, its oxygen-contain- ronment provided by cement pore solution (in the pres-
ing functional groups fancy involving chemical/physical ence of divalent ions) [29, 82, 84, 85].
interactions [20, 24, 75], and then enhancing the bond Table 2 summarizes the dispersion methods of CNMs
strength [73, 76]. Based on these characteristics, it has in the water and cement matrix. According to the pub-
been generally accepted that GO can accelerate cement lished literature, acid treatment and surfactant wrap-
hydration [20, 53, 75, 77, 78], improve the polymerization ping are generally the most used strategies to overcome
Fig. 2 Schematic illustration of electrochemically gathered graphite oxide (OEGO) synthesis. EGO and GIC are the electrochemically gathered GO
and graphite intercalation compounds, respectively [68]. (Copyright 2017 ACS)
Fig. 3 The relative number of published articles of various CNMs used for manufacturing cement composites, rGO is reduced GO. (Data collected
from Google Scholar from 2011 to 2021, total of 14206 published literature)
Table 2 Dispersion methods of CNMs in water and cement matrix

Dispersion methods System Description Ref.
Ultrasonic dispersion Water Ultrasonic waves/energy can cavitate and exfoliate the CNMs. [28, 86, 87]
Acid treatment Water The strong steric hindrance effects can separate CNMs from [38, 65]
Surface modification Water/cement charged ions. [82, 84, 85, 88]
pore solution
Mechanical dispersion Mechanical agitation Cement matrix Applying shearing force created by mechanical friction, colli- [19, 51, 89–91]
Ball milling sion, and crush on CNMs. [52, 92, 93]
Integrated dispersion method Cement matrix The combined usage of the aforementioned methods. [21, 22]
Silica fume or nano-silica Cement matrix Using spherical particles to prevent agglomeration of CNMs. [84, 85, 94–97]
attractions between CNMs [52, 82, 85, 88, 92]. Specifi- Dispersion of CNMs in water
cally, acid can endow charges on the surface of CNMs At present, admixtures are indispensable constituents in
at the cost of some detrimental effects on their struc- modern cement concrete applications [5, 12, 36, 37, 44,
ture [65], while surfactant wrapping can make CNMs 99]. Surface active chemicals, including superplasticiz-
more compatible with water, with the mechanism of ers, shrinkage reducing admixtures, and air-entraining
either charge repulsion or steric repulsion depending surfactants, etc., are prepared in the form of an aqueous
on the molecular structure of surfactant [29, 82, 85, 88]. solution before mixing with cement powder [82, 84, 85,
However, the high ionic concentration of cement pore 100]. Along with this idea, the preparation of uniform
solution (high alkalinity and di-covalent Ca ions), could aqueous dispersion of CNMs can facilitate their practical
severely screen charge repulsion interaction [84, 98]. applications [9, 101].
Therefore, considering the highly complex electrolyte Currently, the dispersion methods of CNMs in water
environment of pore solution in cement hydration, the mainly include mechanical shearing and ultrasonica-
achievement of uniform dispersion of CNMs in cement tion, and surface physiochemical modification [19, 91],
matrix is still very challenging. Since CNMs are typi- as presented in Table 2. For a given material, the disper-
cally dispersed in water before mixing with cement, this sion capability of shearing is mainly dependent on the
review work summarized CNMs dispersion in water, shearing stress, which in turn, are determined by the
cement pore solution, and cement matrix, separately, shearing rate and viscosity of the dispersion [51, 52, 89].
to clarify the main mechanism and related colloidal Since the viscosity of CNMs dispersion is typically in
behavior in each step. the same range of water [102], the maximum shearing
stress and dispersion quality that can be realized is very because of the high ionic strength resulted from cement
limited. Ultra-sonication is a process based on cavita- dissolution.
tion (about 200 W and the frequency of 30 kHz), with Another surface modification method is to wrap CNMs
high local energy, and has been extensively employed with surfactants [37, 82, 84, 85, 88, 100]. Broadly, the sur-
for CNMs dispersion [21, 22, 28]. The effectiveness of factants can be divided into categories of anionic [82],
ultra-sonication can be optimized by a proper combi- cation [106], and neutral type [82], all of them have been
nation of sonication power and sonication time [19, 21, studied for CNMs dispersion. As matter of fact, organic
22]. Note that, because of the high cavitation energy, admixtures, including water-reducing admixtures,
the crystal structure and aspect ratio of CNMs may be air-entraining admixtures, superplasticizers, shrink-
destroyed and reduced, both of which will decrease the age reducing admixtures, are all surfactants that can be
reinforcement efficiency of CNMs [22, 99]. Besides, for potentially employed to disperse CNMs [82, 88, 107].
a given material and sonication power, the dispersion Polycarboxylate superplasticizer (SP), which is currently
quality will be saturated with time, as reported by Cole- the most used surfactant, has been extensively inves-
man et al. [103]. Therefore, proper optimization of son- tigated to disperse CNMs and enhance the stability of
ication conditions is required to further promote the the resulted dispersion upon increasing ionic strength
dispersion quality of CNMs. [82, 85, 88, 100, 107, 108]. As illustrated in Fig. 4, using
To further promote the dispersion quality, CNMs can SP in a GO-cement system can disperse GO nanosheets
be grafted with hydrophilic functional groups, both and cement grains at the same time (Fig. 4a). Similarly, a
physically and chemically [81, 82]. GO, which has been good dispersion quality of graphene in an aqueous solu-
extensively used to modify cement matrix past the last tion can be achieved with the help of SP (Fig. 4b). How-
decade [20, 24, 77, 82, 104, 105], can be considered as ever, it should be noted that the absorbed surfactant itself
graphene that is chemically grafted with a significant could also be stripped off when the ionic strength is high
amount of oxygen-containing groups [64]. CNTs treat- enough [82, 110]. For instance, Zhao et al. [100] reported
ment by strong acid is also commonly used to facilitate that the GO could aggregate again when the Ca ions con-
its dispersion in water [38, 65]. As explained above, centration was reached 1 M (NaOH solution) or higher
such a dispersion method relies on the surface charge [82].
repulsion, which can be easily screened out by ions if Interestingly, the stability of surfactants that are
there is any [20]. This means that even CNMs can be wrapped around CNMs in the various electrolyte has
well dispersed in water after chemical modification, been systematically investigated since more than two
they might still agglomerate when mixed with cement, decades ago in environmental science [80–82, 85, 111],
Fig. 4 Schematic diagram of (a) SP dispersing GO nanosheets and cement grains at the same time [100]. (Copyright 2018 Elsevier). And (b) the
dispersion of graphene by SP [109]. (Copyright 2018 Elsevier)
in which, the agglomeration of particles is one of the 0.01 wt% GO and cement were mechanically stirred for
key research topics. However, the exact chemical struc- about 5 min to obtain a uniform mixture, while they
tures of most SP are generally confidential, blurring the failed to achieve good dispersion when the GO amount
optimization of the CNMs dispersion. Because SP is was 0.06 wt% GO, due to the physical cross-linking and
synthesized for cement property modification through Van der Waal’s forces between GO nanosheets. It is
SP-cement grain interaction, a new surfactant should be almost impossible to dis-entanglement CNMs agglom-
designed and prepared specifically for the CNMs dis- erations just by normal shear mixing apparatus. Recently,
persion. Moreover, the stability of surfactants for CNMs silica fume/nano-SiO2 with extremely small particle size
dispersion still needs to be studied and clarified [85]. As and spherical particles, have been employed to disperse
reported by Birenboim et al. [22], the introduction of CNMs in the cement matrix by a pre-mixing process [84,
surfactants can retard the cement hydration and entrap 85, 97, 105, 107, 113], as illustrated in Fig. 5. Because of
substantial air in cement paste. It has been pointed that the high SSA of CNMs, the effectiveness of using silica
caution should be exercised when using surfactants fume as carriers to disperse CNMs, mainly depends on
in the aqueous matrix, as it can lead to foaming [12, the available surface area of the carriers. For instance,
22]. Therefore, there might be a trade-off between the Kim et al. [115] investigated the effect of silica fume con-
positive effects of CNMs and the negative influences of tent (0-30%, mass by cement) on the dispersion of CNTs
surfactants. in a cement matrix, and found that 20 wt% silica fume
and 0.3 wt% CNTs were mixed for 4 min could facilitate
Dispersion of CNMs in the cement matrix the dispersion of CNTs. We can roughly estimate the
CNMs can also be considered to be an admixture in the maximum concentration of well-dispersed nano-SiO2
form of dry powders, and directly mixed with cement, that can be realized by this strategy as follows. Assum-
similar to silica fume, fly ash, and slags [19, 28, 29, 51, 89]. ing that the silica fume particles with a typical size of
Typically, CNMs are mechanically mixed with cement 50-300 nm can be well separated and completely covered
particles for several minutes to obtain a homogeneous by a single layer of closely compacted nano-SiO2 (with
mixture and then mixed with water and other raw mate- a typical size of 4-20 nm), the concentration of nano-
rials to manufacture cement composites [16, 20, 24]. SiO2 in the cement matrix could reach obtain an optimal
For example, as indicated by Mohammed et al. [112], value. Note that, this method in fact realizes a uniform
Fig. 5 Schematic of GO-SiO2 nanohybrids (GOS) dispersion [105]. (Copyright 2020 Elsevier). b SEM image of the graphene-silica fume dispersion in
cement matrix [114]. (Copyright 2018 Elsevier). And (c) SEM image of GO-silica fume dispersion [84]. (Copyright 2018 Elsevier)
distribution of nano-SiO2 throughout the whole matrix, Dispersion quality assessment

at the cost of local severe agglomeration specifically at Table 3 summarizes the current techniques are adopted
the surface of silica fume. Therefore, such nano-SiO2 can to evaluate the dispersion quality of CNMs in water or
in principle only modify the local chemistry and micro- cement matrix. As can be seen, much evidence reported
structure around silica fume. Also, the pre-mixing time the CNMs dispersion quality in water by techniques of
of silica fume and CNMs is another key factor that affects UV-vis spectroscopy [82, 99], laser particle size analysis
the dispersion of CNMs in the cement matrix. For exam- [9, 84], dynamic light scattering [8, 119], zeta potential
ple, Akarsh et al. [94] and Bai et al. [114] pointed out the [82, 109], optical microscope [82, 85], and SEM obser-
GO-cement and graphene-cement should premix for vation [21, 28, 120, 121]. However, noted that the high
approximately 3 min and 10 min, respectively, to obtain dispersion quality of CNMs in water before mixing with
a uniform mixture. A similar pre-mixing time for nano- cement is not necessarily resulting in high dispersion
SiO2 and CNMs was also reported in other studies [85, quality in the cement matrix.
97, 105]. Because cement is highly heterogeneous, including
To increase the shearing stress significantly, high- multiple phases and pores at multiple scales, the disper-
energy ball milling can be applied [52, 92, 93, 116]. For sion quality of CNMs in a cement matrix is very difficult
instance, Ghosh et al. [117] proposed that the graphene to evaluate [12, 30, 36, 44, 100]. And the extremely low
and cement grains were blended using a planetary ball CNMs concentration (e.g., 0.01-0.1 wt%) typically used
mill via 30 g Zirconia balls, which is an efficient approach further makes this task formidable. SEM equipped with
to obtain a homogenous distribution of graphene with energy dispersive spectrometer (EDS) has extensively
cement grains. Jing et al. [92] used X-ray diffraction been used to characterize the dispersion of CNMs in
(XRD) and scanning electronic microscope (SEM) to ver- cement matrix [21, 28, 43, 122], although it is difficult to
ify this hypothesis. A similar beneficial role of ball milling locate and even confirm that it is indeed CNMs due to
on dispersion graphene was reported in another report the complexity of the hydration products. However, SEM
[89], in which the graphene and cement were dry mixed cannot achieve quantitative characterization of CNMs
for 72 h. Chiranjiakumari et al. [118] using a high-energy dispersion in the cement matrix. The complete evalu-
planetary ball mill method (at 500 rpm for 8 h) to dis- ation of CNMs dispersion and distribution in cement
perse GO in the matrix, and found that adding 0.1 wt% matrix is critically important for the design and optimi-
GO in 100% recycled concrete could be an alternative zation of the CNMs-cement interaction, and effectively
way to achieve sustainability in the construction industry. promotes the effectiveness of CNMs. Recently, Cui et al.
As discussed above, ball milling provided an alterna- [99] found that the UV-Vis absorbance value of the GO
tive method for dispersing CNMs in a cement matrix and suspension increased from 0.72-0.95 when ultrasonica-
showed great practical significance to fabricate CNMs- tion energy increased from 15% to 60%, indicating that
cement composites [93]. Note that, the ball-milling higher ultrasonication energy resulted in a higher degree
process can also result in cement powder fining, which of GO dispersion. Additionally, they found that the ratio
increases the reactivity of cement particles [92, 116]. of Raman intensity of D band G band (ID/IG ratio) rose
Thus, cautions should be taken when evaluating the true with increasing sonication energy. Therefore, the energy
effects of CNMs on the performance of the obtained input of 30% was selected to obtain a balance between
cement composites. the GO dispersion [99]. This provides new possibilities
Table 3 Techniques are adopted to evaluate the dispersion quality of CNMs in suspension or cement matrix
Methods System Description Ref.
UV-vis spectroscopy Suspension Employing the Beer-Lambert Law to calculate the content of CNMs [4, 82, 99]
according to the absorbance.
Laser particle size Smaller particle size indicates better dispersion [9, 84]
Dynamic light scattering [8, 119]
Zeta potential Higher zeta potential value (absolute value) means better dispersion [82, 109]
Optical microscope Suspension/ Assessment of dispersion based on directly observed dimensions [82, 85]
SEM cement matrix [21, 28, 120, 121]
Transmission electron microscope [22, 32, 87]
X-ray photoelectron spectroscopy [22, 24, 86, 105, 107, 119]
Raman spectrum [86, 120]
for a more refined characterization of CNMs dispersion subsequent mechanical and durability properties of hard-
in the cement matrix. However, such analysis is severely ened cement composites.
limited by the resolution of the laser point. Again, hydra- Despite the substantial research effort devoted to ful-
tion products including ettringite (AFt), monosulfate filling the nucleation effect potential of the CNTs, pre-
(AFm), and calcium hydroxide (CH), all have their own vious reports of CNTs accelerate cement hydration are
shape factor (geometrically, AFt has nano-needle shape, somewhat contradictory [22, 24, 27, 38], with some stud-
while AFm and CH have nano-plate shape) [123, 124], ies demonstrating an obvious acceleration effect [20, 24]
which make it very difficult to distinguish them from and others no effects or even retardation [27, 38], as illus-
the added CNMs. For instance, Meng et al. [125] used trated in Fig. 6. For instance, an investigation was con-
SEM to locate the distribution of graphene nanoplates, ducted by Sobolkina et al. [38], who indicated that the
which as matter of fact, could also be AFm. Therefore, the addition of either 0.25 wt% H NO3-oxidized CNTs hardly
employment of elemental mapping or other complemen- affects C3S hydration, and they argued that the insig-
tary techniques is necessary to confirm that the focused nificant effect was mainly due to the limited adsorption
materials under SEM are indeed CNMs. sites present on CNTs surface (Fig. 6a). It was hypothe-
sized that some functional groups on the CNTs surface
Influence of CNMs on the performance of cement or other CNMs may stimulate cement hydration as the
composites generation of additional calcium silicate hydrate (C-S-H)
Properties of fresh cement composites [38]. Tafesse et al. [27] reported that pure CNTs are not
In this review work, the main properties of interest capable of activating or delaying cement hydration, based
of fresh cement mixture including hydration kinetics on the results of nonevaporated water (Fig. 6b), rather,
and rheology properties, both of which will affect the they only provide nano-filler effect in cement composites.
Fig. 6 a Isothermal calorimetry results for the C3S pastes [38]. (Copyright 2016 Wiley). b Hydration results were determined indirectly from the
nonevaporated water [27]. (Copyright 2019 Elsevier). And (c) isothermal calorimeter results for cement paste [24]. (Copyright 2018 Elsevier). SP is a
polycarboxylate superplasticizer
In contrast, Jung et al. [28] reported that the surface of repulsion [29, 44, 97, 107], which prevent the agglomera-
the dispersed CNTs can contribute to precipitate cement tion of cement grains. As provided in Fig. 7, Li et al. [135]
hydrates. These inconsistent findings may be attributed found that the introduction of SP significantly decreased
to the dispersion quality and surface chemical affinity of the yield stress (~80%) and minimum viscosity (~70%) of
CNTs. Note that the high surface area of CNTs cannot cement pastes (w/c=0.24) in the presence of graphene
guarantee seeding effect, as reported by many groups (at a dosage of 0.75 wt%). However, in the presence of SP,
[27, 38, 126]. It has been generally accepted that GO can especially the content over 0.75 wt%, the admixing gra-
accelerate cement hydration because of the rich oxygen- phene can hardly influence the yield stress and minimum
containing functional groups on its surface [20, 22, 100]. viscosity of cement pastes. Note that, the admixed CNMs
A recent study found the incorporation of 0.025 wt% GO may affect the compatibility between cement materi-
resulted in an earlier heat flow peak [24], as illustrated als and surfactants thus affect the rheological properties
in Fig. 6c. A similar accelerating effect of GO on cement of cement mixture [29, 136]. In addition, a few stud-
hydration was found in other studies [79, 127], in which ies reported that CNMs can lubricate solid particles in
the introduction of 0.025-0.10 wt% GO can significantly cement composites, which improved the flowability of
increase the heat flow of cement composites. Unfortu- the mixture [22, 29, 125]. Such knowledge gaps constrain
nately, direct evidence for the seed effects of CNMs is the wider acceptance of CNMs in developing cementi-
still missing, which will be elaborated in the following. tious composites and drive the need for further research
Generally, adding CNMs to the cement matrix can lead to advance the understanding.
to an improvement of viscosity (decreased workability),
since the super-high SSA of nanoparticles requires more Properties of hardened cement composites properties
water for surface wetting [5, 31, 36, 44, 100]. The low vis- Mechanical strengths
cosities of the fresh mixtures have a negative influence Mechanical properties of cementitious composites are
on the mixing and casting process and then affect the generally regarded as the most important performance
final mechanical and durability properties [5, 9]. Accord- in practical applications [12, 30, 31, 36, 44, 101]. Dur-
ing to the rheological parameters of paste obtained from ing the past decades, it had been generally accepted that
the Bingham curve [128], the plastic viscosity (η) of the admixing a small dosage of CNMs to cement can result
cement mixture (w/c=0.36) incorporating 0.03 wt% GO in remarkable improvement in the mechanical strengths
(by weight of cement) was approximately 40% higher (e.g., compressive, flexural, and tensile strength) [20, 28,
than that of the plain cement. Similarly, the admixing 0.3 32, 114, 128, 137].
wt% CNFs resulted in increased plastic viscosity of paste Table 4 illustrates the experimental findings collected
(w/c=0.20) by approximately 35% [29]. from the published reports related to the enhancement of
Surfactants may be an ideal candidate to overcome this CNMs to the mechanical strengths. As can be seen, GO
issue because of their steric hindrance and electrostatic (generally 0.01-0.10 wt%, by weight of cement) is typically
Fig. 7 Influence of CNMs on the rheology properties of fresh mixtures: a yield stress and b viscosity [22, 29, 97, 128–134]. SP is standing for
polycarboxylate superplasticizer
Table 4 Improvement of CNMs to mechanical properties of cement-based materials cured at 28 days

Matrix CNMs types w/c Increment in mechanical strengths Ref.
(by weight of cement)
Compressive Flexural Tensile
Paste Graphene (0.05 wt%) 0.35 3-8% 15-24% - [138]

Paste Graphene (0.025 wt%) 0.40 14.9% 23.6% 15.2 [139]
Paste Graphene (2 wt%) 0.38 -33.3% [140]
Paste GO (0.05 wt%) 0.35 29.0% - - [20]
Paste GO (0.01 wt) 0.30 10.0% 15.6% - [79]
Paste GO (0.03 wt) 0.30 20.1% 27.3% -
Paste GO (0.05 wt) 0.30 27.5% 30.7% -
Paste CNFs (0.1 wt%) 0.485 - 20% - [34]
Paste CNTs (0.15 wt%) 0.40 14.3% 3% - [141]
Mortar GO (0.022 wt%) 0.42 34.10% 30.37% 33.0% [88]
Mortar GO (0.1 wt%) 0.48 27.7% - - [142]
Mortar Graphene (0.05 wt%) N.A. 8.3% 15.6% [143]
Mortar GO (0.15 wt%) 0.35 13.7% 14.5% [94]
Mortar GO (0.01 wt%) 0.37 13.4% 51.7% 47.0% [80]
Mortar GO (0.03 wt%) 0.37 38.9% 60.7% 78.6%
Mortar GO (0.05 wt %) 0.37 47.9% 30.2% 35.8%
Mortar CNTs (0.3 wt%) 0.40 -2.7% - - [43]
Mortar CNTs (0.5 wt%) 0.60 -1.8% - -
Mortar CNFs (0.1 wt%) 0.485 6.15 - - [34]
Concrete CNFs (0.30 wt%) 0.20 60.0% 10.1% 55.0% [29]
Concrete CNTs (0.002 wt%) 0.23 -1.1% - - [28]
Concrete CNTs (0.005 wt%) 0.23 5.5% - -
Concrete CNTs (0.008 wt%) 0.23 -0.8% - -
Concrete CNTs (0.01wt%) 0.23 -4.9% - -
Concrete CNFs (0.1 wt%) 0.51 8.13% - - [34]
Concrete CNFs (0.10 wt%) 0.51 6.16% - - [144]
Concrete Graphene (0.30 wt%) 0.20 40% 59% - [125]
Concrete Graphene (0.10 wt%) 0.16 62.25 9.25 - [145]
used to manufacture cement paste and cement mortar, a large number of flower-like hydration crystals were
while CNFs and CNTs are generally used to fabricate grown on GO sheets (Fig. 8b), this phenomenon is pos-
cement concrete, especially used to prepare ultra-high- sibly explained by the template effect of GO, inducing
performance concrete. For improving the compressive hydrates growth in a specific space [79, 146]. Notably, the
strength of cement-based materials, the addition of GO is nucleation effect is a prerequisite for the template effect
more effective than other CNMs, while CNTs and CNFs and this phenomenon merely occurs in a cement matrix
seem more effective for improving the flexural and tensile incorporating GO sheets, which has been observed by
strengths of cement-based materials. many reports [39, 46, 79, 80]. ii) The nano-filler effect
As illustrated in Fig. 8, the reinforcement mechanisms reduces the porosity and refines the microstructure [5,
proposed by the current literature include i) acting as a 88]. A recent study was carried out by Konstantopou-
nucleation site to promote cement hydration [20, 22, los et al. [147], who showed that introducing 0.5 wt%
24]. For instance, Sobolkina et al. [38] indicated that CNTs resulted in higher density hydrated phases and
the CNMs with high SSA and rich in oxygen-containing lower total porosity, this phenomenon was explained by
functional groups on their surfaces have a nucleation nanoindentation as enhanced C-S-H connectivity in the
effect on early C3S hydration, as illustrated in Fig. 8a. porous network. Besides, Birenboim et al. [22] found that
Also, Birenboim et al. [22] reported that admixing a a dense microstructure was achieved with the addition of
low concentration of GO (<0.05 wt%) can increase the 0.03 wt% GO, mainly due to the admixed GO nanosheets
compressive strength of paste by 40%, mainly due to the that can act as a nanofiller that refined the microstruc-
nanosize of GO act as a nucleation site. Interestingly, ture (Fig. 8c). However, considering the small number of
Fig. 8 Reinforcement mechanisms of CNMs in cement matrix: a nucleation effect [38]. (Copyright 2016 Wiley). b template effect [79]. (Copyright
2014 Elsevier). c nano-filler effect [22]. (Copyright 2019 Elsevier). And (d) crack-bridging effect [30]. (Copyright 2019 Elsevier)
CNMs that are utilized, typically less than 0.1 wt%, purely observed to be attached on CNMs. Note that, this phe-
physical filler effects are probably negligible. And iii) the nomenon can be also induced by the growth of hydration
bridging effect to inhibit microcracks propagation [8, 27– products far away from CNMs, and CNMs are merely
29]. Silvestro et al. [91] indicated that the incorporation passively embedded inside. Recently, we have employed
of 0.1 wt% CNTs increased the 28-d compressive and CNTs sponges, with unique nano-pores microstruc-
tensile strengths of a cement paste by up to 30% and 50%, ture, as a platform to in-situ separate pore solution from
respectively. The microcracks were eliminated with the cement grains [71]. The experiments directly prove that
addition of CNTs and CNFs [148, 149], and the admix- CNT with and without strong acid treatment are all inert
ing CNMs plays a dominant role in enhancing the flex- for cement hydration, and there is no seed effect.
ural strength and tensile strength of cement composites
because of their larger aspect ratio (Fig. 8d), as discussed Durability
in section 2. Durability is critical to guarantee the reliability and sta-
Recent work was conducted by Xu and Shi et al. [20], bility of cement composites [5, 12, 31, 36, 37, 101]. Typi-
who found that the admixing 0.02 wt% GO promoted cally, their durability is evaluated in terms of transport
cement hydration to generate Si-rich phases (tober- properties and chemical resistance [30, 37]. It is an issue
morite-like hydrate) and Ca-rich hydrates (jennite-like attracting wide interest in the application of cementitious
structure), instead of ordinary C-S-H gel. This seems to composites as it relates to the safety, service life, and
provide a new possibility to explain the possible mecha- maintenance costs [30, 150–153]. Currently, the dura-
nisms of GO-reinforced cement composites. Note that bility of CNMs reinforced cement composites has not
the reported experimental evidence mainly comes from been sufficiently studied, compared to the comprehensive
SEM images of fractures cement composites samples, studies concerning their mechanical properties. This sec-
where CNMs are exposed and hydration products can be tion summarized the findings brought out by CNMs in
the durability of cement composites in recent literature, Chemical degradation of cement-based materials gen-
including transport property and chemical degradation. erally includes sulfate attack, carbonation, and acid attack
Transport properties of cement composite reflect its [12, 30, 36, 37]. As discussed above, the addition of CNMs
resistance to the ingress of aggressive agents (e.g., water also showed great potential to improve the chemical
and ions, etc.) to pass through inside [12, 30, 36, 150, resistance for cement composites. For example, the intro-
151], which can be improved by introducing well-dis- duction of 0.03 wt% GO reduced the carbonation depth
persed CNMs [122, 152]. For instance, an investigation due to the movement of CO2 molecules into the cement
was carried out by Qureshi et al. [153], who reported matrix was restricted by GO, that is, the reduction of car-
that the maximum water vapor adsorption at 98% relative bonation depth of GO-reinforced cement composites is
humidity increased up to 2% in the 0.06% GO-cement related to the reduced porosity [53, 154]. Also, Long et al.
composites, suggesting additional C-S-H gel was formed [53] found that the introduction of 0.2 wt% GO could
in the cement composites, which can induce a denser reduce the carbonation depth by approximately 40%
microstructure (see Fig. 9). A similar result has been after 28 days, mainly due to the reduced porosity and
observed by others [53, 112], who found that the water refined pore structure, as presented in Fig. 10a. Accord-
absorption and gas permeability of a cement composite ing to Mohammed et al. [155], who reported that a con-
could be reduced by 10-20% with the addition of GO. siderable decrease (from 11 mm to 2 mm) of carbonation
Similar to the role of GO in the cement matrix, CNTs or depth in a cement specimen incorporating 0.06 wt% GO
CNFs possess the nanofiller effect and bridging effect to after 15 months, this result has attributed the benefit to
improve the microstructure of cementitious materials the increased air content and the decreased mesopore
[28–30, 122]. volume (see Fig. 10b and c). Similarly, a recent study was
Fig. 9 Properties of cement composites with the addition of GO: a mass loss b pore size distribution c SEM images of mixture with 0.06 wt% GO,
and d magnification of black rectangle indicating the surface growth nature of flake structures and AFt [153]. (Copyright 2019 Elsevier)
Fig. 10 a Carbonation depth of GO-cement composites, b porosity and pore structure, c changes of cement composites with different GO
contents [53]. (Copyright 2018 Elsevier). d Carbonation depth of cement composites with 0.06 wt% GO, and e images of cement pastes after
carbonation [155]. (Copyright 2018 Elsevier). Note: Carbo is carbonation and the GO content is by weight of cement
carried out by Li et al. [47], who reported that the weight SSA and abundant hydrophilic functional groups, ena-
loss of a paste specimen incorporating CNTs decreased bling it to perform better in improving the durability of
by 13.3%. A similar beneficial role of CNTs or CNFs on cement-based materials. Currently, although the con-
the chemical resistance of cement composites was also sensus is that the durability of cement-based materials
found in other studies and attributed this benefit to the strongly relies on both strength and microstructure, the
refinement microstructure [21, 22, 27–29]. fundamental mechanisms underlying the durability dam-
Overall, the addition of CNMs has demonstrated a age of CNMs-reinforced cement-based materials are not
promising durability performance for cement materials. fully unraveled. To this end, more in-depth studies should
Compared with CNTs or CNFs, GO has a much higher be explored in the future to verify this hypothesis.
Conclusions and remaining challenges harm the setting time and workability of the mix-
Over the past decade, the addition of a small dosage of tures, which is not conducive to the later transpor-
CNMs has demonstrated great potential to improve the tation, casting, and compaction process. Fortunately,
mechanical and durability properties of cement com- this may be compensated by employing some SCMs,
posites. We summarized the relevant publications in the such as fly ash.
last decade (from 2011 to 2021), and the main findings 5) At present, the research of CNMs-engineered
and remaining challenges identified from the literature cement composites is a booming field and there are
review can be drawn as follows: many handicaps to be overcome. The admixing an
extremely low concentration of CNMs has a positive
1) The dispersion quality and distribution of CNMs in influence on the mechanical strengths of cement-
the cement matrix are the keys to understand their based materials, on the premise of effective disper-
roles in the cement matrix. Although previous stud- sion. More attention should be paid to investigate the
ies on the admixed CNMs have achieved some sat- effects of various CNMs on the formation of multiple
isfactory achievements in terms of reinforcement cement hydrates. Additionally, CNMs demonstrate
efficiency [20, 22, 29, 88, 104, 156], the effective great potential to develop smart cement composites
dispersion of CNMs in the cement matrix is still a in the future.
top challenge. Also, semi-quantitative or quantita-
tive evaluation of the dispersion and distribution of
CNMs in cement composites faces great challenges,
which constrains their feasibility to be widely utilized
Abbreviations
in the construction industry. SCMs: Supplementary cementitious materials; CNMs: Carbon-based nanoma-
2) It has been generally accepted that the addition terials; CNTs: Carbon nanotubes; CNFs: Carbon nanofibers; G: Graphene; GO:
of GO can accelerate cement hydration, where Graphene oxide; 1D: One-dimensional; 2D: Two-dimensional; ITZ: Interfacial
transitional zone; OEGO: Electrochemically gathered graphite oxide; EGO:
admixed GO mainly demonstrated the nanofiller Electrochemically gathered graphene oxide; GIC: Graphite intercalation com-
and hydration template roles. In addition, the nega- pound; SP: Polycarboxylate superplasticizer; SSA: Specific surface area; AFt:
tively charged GO could consume Ca ions, thereby Ettringite; AFm: Monosulfate; CH: Calcium hydroxide; C-S-H: Calcium-Silicate-
Hydrate; SEM: Scanning electron microscopy; TEM: Transmission electron
affecting the degree of polymerization of the cement microscopy; XRD: X-ray diffraction; EDS: Energy dispersive spectrometer.
hydrates. However, direct evidence is still very
limited, more detailed investigations need to pro- Acknowledgments
The authors would like to thank Mr. Mingchao Ren for his assistance in data
ceed to investigate the influence of admixed GO on collection.
the formation of cement hydrates. Especially the
cement hydration lasts for a long time and a variety Authors’ contributions
Dong Lu: Data processing, Writing-Original draft preparation, and Writing-
of hydrates are produced at different times, and how Reviewing and Editing. Jing Zhong: Conceptualization, Methodology, Supervi-
(when) the admixed GO affects cement hydration is sion, Writing- Reviewing and Editing. The authors read and approved the final
still needs to be further in-depth studied. manuscript.
3) Pure CNTs or CNFs are generally not capable of acti- Funding
vating or delaying the hydration products, rather, This work was supported by the National Natural Science Foundation of China
they offer a nanofiller and cracking-bridging capabil- [52073073]. The findings and conclusions reported in this article only reflect
the view of the authors and do not reflect the view of the above entities.
ity in cement composites. Interestingly, it has been
found that the CNTs rich in oxygen-containing func- Availability of data and materials
tional groups demonstrated the potential to promote All data generated or analyzed during this study are included in this article.
cement hydration. Overall, the admixed CNTs that
accelerated the cement hydration have not yet been Declarations
unanimously agreed upon. Although previous stud- Competing interests
ies claimed that the nucleation effect of the admixed The authors declare that they have no known competing financial interests
CNMs in the cement hydration, direct evidence is or personal relationships that could have appeared to influence the work
reported in this paper.
still missing. Note that recently, we have utilized
CNTs sponge as a platform to investigate the true Author details
1
effects of CNT on the growth of cement hydration School of Civil Engineering, Harbin Institute of Technology, 73 Huanghe
Road, Harbin, Heilongjiang 150090, P. R. China. 2 Key Lab of Structures Dynamic
products, and the results indicate that CNT with and Behavior and Control of the Ministry of Education (Harbin Institute of Technol-
without acid treatment have no seed effects. ogy), Harbin 150090, P. R. China.
4) For the fresh mixtures, the introduction of CNMs
results in higher viscosity, that is, the admixed CNMs
Received: 11 September 2021 Accepted: 21 October 2021 hardening properties of cement-based materials. Construction Building
Materials, 263. https://doi.org/10.1016/j.conbuildmat.2020.120226
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