Composites: Part A 70 (2015) 6981

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Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa

Review

Review of nanocarbon-engineered multifunctional cementitious

composites
Baoguo Han a,, Shengwei Sun b, Siqi Ding a, Liqing Zhang a, Xun Yu c, Jinping Ou a,b,
a
School of Civil Engineering, Dalian University of Technology, Dalian 116024, China
b
School of Civil Engineering, Harbin Institute of Technology, Harbin 150090, China
c
Department of Mechanical & Energy Engineering, University of North Texas, Denton, TX 76203, USA

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

Article history: As structural materials, cementitious materials are quasi-brittle and susceptible to cracking, and have no
Received 27 August 2014 functional properties. Nanotechnology is introduced into cementitious materials to address these issues.
Received in revised form 3 December 2014 Nano materials, especially nano carbon materials (NCMs) were found to be able to improve/modify the
Accepted 5 December 2014
mechanical property, durability and functional properties of cementitious materials due to their excellent
Available online 19 December 2014
intrinsic properties and composite effects. Here, this review focuses on the recent progress of fabrication,
properties, and structural applications of high-performance and multifunctional cementitious composites
Keywords:
with NCMs including carbon nanobers, carbon nanotubes and nano graphite platelets. The improve-
A. Discontinuous reinforcement
A. Smart materials
ment/modication mechanisms of these NCMs to composites are also discussed.
B. Physical properties Crown Copyright 2014 Published by Elsevier Ltd. All rights reserved.
B. Microstructures

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 69
2. Brief introduction to three types of NCMs used for fabricating NFCC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 70
3. Dispersion of NCMs in cementitious composites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 70
4. Properties of NFCC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
4.1. CNTs/CNFs enhanced/modified cementitious composites. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
4.1.1. Mechanical properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
4.1.2. Electrical and sensing properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 71
4.1.3. Other properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 72
4.2. NGPs enhanced/modified cementitious composites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
5. Characterization methods for NFCC . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
5.1. Characterization methods of dispersion of NCMs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 73
5.2. Characterization methods of performances of composites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
6. Enhancement/modification mechanisms of NCMs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
6.1. Enhancement/modification mechanisms of CNTs/CNFs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
6.2. Enhancement/modification mechanisms of NGPs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
7. Structural applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
8. Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79

Corresponding authors. Tel./fax: +86 411 84780087.

E-mail addresses: hanbaoguo@dlut.edu.cn (B. Han), oujinping@hit.eud.cn (J. Ou).

http://dx.doi.org/10.1016/j.compositesa.2014.12.002
1359-835X/Crown Copyright 2014 Published by Elsevier Ltd. All rights reserved.
70 B. Han et al. / Composites: Part A 70 (2015) 6981
1. Introduction
Cementitious materials are the most commonly and widely
used construction materials for various types of infrastructures.
However, cementitious materials are in general very brittle, and
characterized by low tensile strength and low strain to failure
[1]. Since macroscopic steel bars were used to reinforce the cemen-
titious materials, the size of the reinforcing llers has diminished
from macro scale to micro even nano scale with the development
of nanotechnology. The addition of these tiny llers not only
improves mechanical properties and durability of cementitious
materials, but also endues them with such functionalities as elec-
trical, thermal and electromagnetic properties [2,3]. For example,
the fracture toughness of cementitious composites can be
enhanced by 400% when nano-ZrO2 is used as llers [4]. An addi-
tion of 5% nano-Al2O3 can increase the elasticity modulus of
cementitious composites by 143% [5]. The electrical resistance of
cementitious composites can be decreased by 45% with 5% nano-
Fe2O3 [5]. Nano-TiO2 can endow cementitious materials with the
photocatalytic effect to decompose both organic pollutants and
oxides such as NO, NO2 and SO2 [6]. Moreover, due to their remark-
able mechanical, electrical and thermal properties, excellent nano-
scale effects, low density, and excellent chemical and thermal
stability, nano carbon materials (NCMs) offer the possibility to
develop a new generation of tailored, high-performance, and mul-
tifunctional cementitious composites[5,79]. Extensive research
endeavors demonstrated the potential of various NCMs including
carbon nanobres (CNFs), carbon nanotubes (CNTs) and nano
graphite platelets (NGPs) for enhancing/modifying cementitious
materials [1015]. For example, Li et al. observed that an addition
of 0.5 wt.% CNTs can improve the exural, compressive strength
and the failure strain of the composites by 25%, 19% and 27%,
respectively [11]. Raki et al. reported that CNTs can improve the
Vivtorinox hardness of the early hydration of composites by
600%, the Young modulus by 227% and the exural strength by
40% [7]. Gao et al. found that the compressive strength of compos-
ites with 0.16 wt.% CNFs is 42.7% higher than that of the plain
cementitious materials [12]. Huang obtained a maximum increase
of 82% in the exural strength by adding NGPs into cementitious
materials [13]. NCMs achieve the enhancement effect by nucle-
ation, increasing the amount of CSH gel of high hardness,
improving pore structures, controlling nanoscale cracks, improving
the early strain capacity and reducing autogenous shrinkage of
cementitious composites [514]. These mechanisms would also
improve the durability of the cementitious materials [15]. In addi-
tion, due to their excellent electrical, thermal and electromagnetic
properties, NCMs can impart electrical, thermal, electromagnetic
and sensing properties to cementitious materials [13,14].
During the past decade, considerable research effort has been
directed towards the development of cementitious composites
with NCMs, and many innovative achievements have been
gained in both development and application of the NCMs lled
cementitious composites (NFCC). The aim of this paper is to
Table 1
Properties of NCMs [1,13,1726].
Property CNTs
MWCNTs SWCNTs
Elastic modulus/TPa 0.31 1 0.40.6
Strength/GPa 1060 50500
Electrical resistivity /lX cm 550
Dimensions Diameter: 230 nm Diameter: 0.753 nm
Length: 0.150 lm Length: 150 lm
Surface area/m2/g >400
Aspect ratio 1000
provide a systematical review on major progresses and advances
in the fabrication, properties and mechanism, and structural appli-
cations of NFCC.
2. Brief introduction to three types of NCMs used for fabricating
NFCC
CNTs are allotropes of carbon with a hollowly cylindrical nano-
structure. They are generally a few nanometers in diameter and
several microns in length. According to the number of rolled layers
of graphene, CNTs are categorized as single-walled CNTs (SWCNTs)
and multi-walled CNTs (MWCNTs) [16]. Like CNTs, CNFs are also
the quasi-one-dimensional carbon material, and their diameters
are between those of CNTs and carbon bers (CFs). The representa-
tive properties of CNTs and CNFs are listed in Table 1. NGPs are car-
bon-based conductive nano-particles made from graphite.
Graphene oxide (GO) is a single layer of NGPs that have been oxi-
dized to intersperse the carbon layers with oxygen molecules. The
structures of NGPs are two-dimensional platelets consisting of a
few to several graphene layers with an overall thickness in nano-
meter scale and the particle diameter ranging from submicron up
to 100 lm [13,17,18]. Typical properties of NGPs are also given
in Table 1.
3. Dispersion of NCMs in cementitious composites
Because the strong Van der Waals forces cause the agglomera-
tion of the nano-particles, a key issue in fabricating high-quality
NFCC is to homogeneously disperse NCMs in cementitious materi-
als. Poor dispersion will lead to the formation of defects in the
matrix and limit the nano-enhancement/modication effect [27].
A lot of research work has been done to improve the dispersion
of NCMs in the cementitious composites. Commonly, there are
two types of methods used to disperse NCMs. One method is to
mechanically separate the NCMs by adopting ultrasonic [28
39,4155,5763,6572,7476], ball milling [56,77]or high-shear
mixing technologies. The other method chemically alters the sur-
face of the NCMs by using covalent [11,36,59,61,74]or noncovalent
modication approaches [35,36,4052,54,55,5873,75,76]. More-
over, the mechanical methods are often used in combination with
the chemical methods [10,14,2934].
Recently, researchers have proposed some novel approaches to
solve the dispersion issue of NCMs. The primary approach is to
adopt commonly used water reducing admixtures (including plast-
icizers and superplasticizers) as surfactants. The research at the
National Research Council Canada has shown that a small amount
of CNTs can be dispersed by ultrasonication in the water contain-
ing 5% superplasticizer [14]. Shah et al. also achieved an effective
dispersion of MWCNTs with different lengths and concentrations
in cementitious materials by applying polycarboxylate-based
superplasticizers [3739]. Yazdanbakhsh et al. performed a
three-dimensional simulation study, and stated that only when
CNFs NGPs
1 (in-plane)
2.77.0 1020
55 50 (in-plane)
Diameter: 50200 nm Diameter: 120 lm
Length: 50100 lm Thickness: 30 nm
200 2630
100500 50300
 B. Han et al. / Composites: Part A 70 (2015) 6981 71

cement particles are also distributed homogeneously without any
agglomeration, the degradation effect of cement particles on the
homogeneous distribution of CNTs within cementitious materials
is negligible [78]. Meanwhile, Han et al. pointed out that the effec-
tive dispersion of superplasticizers to CNTs/CNFs can be contrib-
uted to their double-dispersion effect on CNTs/CNFs and cement
particles [19]. Huang also employed superplasticizer to obtain a
proper dispersion of NGPs in cementitious materials [13]. There-
fore, the dispersion of NCMs with water reducing admixtures is
an excellent method for fabricating NFCC without adding any addi-
tional dispersants that impair the hydration or mechanical proper-
ties of composites. However, this method only can improve the
dispersion effect to some extent because of the limit of dispersion
capability for water reducing admixture, and it needs high energy
consumption due to use of ultrasonic treatment. Nasibulin et al.
put forward a new method to solve the dispersion problem of
CNTs/CNFs, which is to make CNTs/CNFs and cement/mineral
admixture a whole by in-situ growing CNTs/CNFs on the cement,
mineral admixture particles or sand [14,7986]. Generally, the dis-
persion of NCMs in cementitious composites is still a critical issue.
It is necessary to nd more simple, repeatable, large-scale and low-
energy consumption methods for distributing NCMs in cementi-
tious composites without altering the manufacturing process of
composites.
4. Properties of NFCC
4.1. CNTs/CNFs enhanced/modied cementitious composites
4.1.1. Mechanical properties
Since early investigations showed that CNTs have strong effect
on the hydration process and hardness of cementitious composites
[35], lots of researches have been done to ascertain mechanical
properties of CNTs/CNFs lles cementitious composites. These
researches and their results are summarized in Tables 2 and 3.
The mechanical properties of NFCC are closely related to not only
the type, the concentration, the surface condition and the disper-
sion quality of CNTs/CNFs, but also the composition of cementi-
tious materials. As shown in Tables 2 and 3, the observed best
performance enhancement of NFCC include a 300% increase in
compressive strength [25], a 34.28% increase in tensile strength
[91], a 269% increase in exural strength [44], a 270% increase in
fracture toughness [41], a 14% increase in fracture energy [87,88],
an over 600% improvement in Vickerss hardness at the early ages
of hydration [35], a 2200% increase in deection [74], a 130%
increase in ductility [44], an over 430% improvement in resilience
[23]and a 227% increase in Youngs modulus[40]. In addition, it
should be noted that the addition of CNTs/CNFs also changes the
mechanical constitutive relations of composites (as shown in
Fig. 1(b) and (c)).
4.1.2. Electrical and sensing properties
The addition of CNTs/CNFs decreases the electrical resistivity of
cementitious composites to nearly 1 X cm and increases their elec-
trical conductivity by maximally about 8 orders of magnitudes
against the plain one (as shown in Fig. 2a)) [56]. Just like the
mechanical properties of cementitious composites, their electrical
conductivities are also strongly dependent on the type, the concen-
tration, the surface condition and the dispersion quality of CNTs/
CNFs, and the composition and water contents of cementitious
materials [14,19,46,97104]. Meanwhile, the CNTs/CNFs
enhanced/modied cementitious composites also exhibit sensitive,
stable and repeatable response of electrical property to external
force or deformation [14,19,9799]. Recently, much effort has been

Table 2
Enhancement of CNTs to mechanical properties of cementitious materials.

Mechanical properties Enhancement in properties Concentration of CNTs Researchers

SWCNTs MWCNTs
Hardness 600% 2 wt.% Makar et al. [35]
177% 0.1 wt.% Ibarra et al. [40]
Tensile strength 34.28% 0.3 wt.% Ludvig et al. [91]
19% 0.5 wt.% Hunashyal et al. [92]
Tensile modulus 70.9% 0.5 wt.% Hunashyal et al. [92]
Compressive strength 19% 0.5 wt.% Li et al. [11]
70% 0.05 wt.% Yakovlev et al. [93]
11.03% 0.02 wt.% Keriene et al. [48]
50% 0.0450.15 wt.% Cwirzen et al. [36]
29.5% 0.2 wt.% Luo et al. [62]
25% 0.5 wt.% Collins et al. [45]
1020% 0.5 wt.% Musso et al. [60]
22% 0.1 wt.% Bharj et al. [57]
25% No given Hlavcek [87]
200% No given Nasibulin et al. [94]
30% 0.15 wt.% Kim et al. [64]
Flexural strength 25% 0.5 wt.% Li et al. [11]
10% 0.0450.15 wt.% Cwirzen et al. [36]
11.23% 0.004 wt.% Keriene et al.[48]
34% 0.5 wt.% Musso et al. [60]
43.75% 0.75 wt.% Hunashyal et al. [58,92]
269% 0.2 wt.% Al-Rub et al. [44]
35.45% 0.2 wt.% Luo et al. [62]
25% 0.048 wt.% and 0.08 wt.% Konsta-Gdoutos et al. [49]
Fracture toughness 149.32% 0.5 wt.% Luo et al. [63]
Ductility 130% 0.2 wt.% Al-Rub et al. [44]
28% 0.5 wt.% Hunashyal et al. [92]
Fracture energy 14% No given Hlavcek [87]
Modulus of toughness 154% 0.04 wt.% Al-Rub et al. [44]
Fracture modulus 34.7% 0.5 wt.% Musso et al. [60]
Critical opening displacement 34.96% 0.5 wt.% Luo et al. [63]
Youngs modulus 45% 0.048 wt.% and 0.08 wt.% Konsta-Gdoutos et al. [49]
50% 0.048 wt.% and 0.08 wt.% Shah et al. [38]
227% 0.1 wt.% Ibarra et al. [40]
72 B. Han et al. / Composites: Part A 70 (2015) 6981

Table 3
Enhancement of CNFs to mechanical properties of cementitious materials.

Mechanical properties Enhancement in properties Concentration of CNFs Researchers

Ductility 35.1% 1.0 vol.% Howser et al. [73]
73% 0.1 wt.% Al-Rub et al. [42]
Resilience 430% 1.0 wt.% Yazdanbakhsh [23]
Stiffness 25% 0.1 wt.% Al-Rub et al. [42]
Deection 34.9% 1.0 vol.% Howser et al. [73]
2200% 0.04 vol.% Peyvandi et al. [74]
Tensile strength 2226% 0.2 wt.% Gay et al. [72]
Compressive strength 300% 0.4 wt.% Nasibulina et al. [25]
21.4% 1 vol.% Gao et al.[95]
42.7% 0.16 wt.% Gao et al. [12]
Flexural strength 82% 0.2 wt.% Tyson et al. [41]
46% 0.04 vol.% Peyvandi et al. [74]
250% 1.0 wt.% wt.% Yazdanbakhsh et al. [70]
60% 0.1 wt.% Al-Rub et al. [42]
45% 0.048 wt.% Shah et al. [71]
Fracture toughness 270% 0.2 wt.% Tyson et al. [41]
Impact resistance 280% 0.04 vol.% Peyvandi et al. [74]
Energy sorption 3400% 0.04 vol.% Peyvandi et al. [74]
Abrasion weight loss 1700% 0.04 vol.% Peyvandi et al. [74]
Modulus of toughness 170% 0.1 wt.% Al-Rub et al. [42]
Peak displacement 150% 0.2 wt.% Tyson et al. [41]
Ultimate normalized capacity 30.7% 1.0 vol.% Howser et al. [73]
Youngs modulus 50% 0.048 wt.% Shah et al. [71]
68% 1.0 wt.% Yazdanbakhsh [23]

(a) Stress-strain diagrams for cementitious (b) Load vs. mid-span deflection relationships for
composites with 0.04% short MWCNT and 0.1% CNTs enhanced/modified cementitious composites
long MWCNT under compression [44] under bending [96]

Fig. 1. Mechanical properties of typical CNTs/CNFs lled cementitious composites. (For interpretation of the references to color in this gure legend, the reader is referred to
the web version of this article.)

done on the sensing behavior (as shown in Fig. 2b)) of cementitious
composites with different types and concentrations of CNTs/CNFs
under different loading types, loading speeds, loading frequencies,
temperatures, humidies (or water contents), etc. [14,19,46,95,97
104].
4.1.3. Other properties
Damping, thermal, electromagnetic interference (EMI) and
other properties of CNTs/CNFs enhanced/modied cementitious
composites were also investigated. For example, Luo observed that
the frequency responses function (FRF) amplitude (i.e. damping
ratio) of composites increases with increased content of MWCNTs
(as shown in Fig. 3a)) [62,105]. Han et al. found that even a very
small dosage of MWCNTs can effectively improve the transport
properties (i.e. water sorptivity) of the composites. The test was
performed by allowing one surface of the specimen to be in contact
with water of 10 mm depth using a circular plexiglas support
through recording the weight of the specimen at xed time inter-
vals (as shown in Fig. 3b))[15]. Yakovlev et al. observed that the
addition of CNTs decreases the heat conductivity of foam concretes
by 20% (from 0.07 W/m K to 0.056 W/m K) [93]. Veedu stated that
the thermal performance of CNTs lled cementitious composites is
at least 35% and 85% higher than that of the CFs lled and the
unmodied ones respectively [65]. Al-Rub et al. found that incor-
poration of CNTs treated by the functional groups (COOH and
OH) produces an improvement to workability of the cementitious
composites [42]. Shukla et al. studied the smoke detection prop-
erty of composites with MWCNTs, and found that the DC transient
studies depict an increase in electrical conductivity when exposed
to smoke [106]. Keriene et al. observed that the non-autoclaved
aerated concrete and the autoclaved aerated concrete with
MWCNTs are more stable during exploitation than those compos-
ites without these additions [48]. In addition, Singh et al. found
that the high value of EMI shielding effectiveness (SE) of MWCNTs
lled cementitious composites is dominated by absorption rather
than reection. An addition of 0.6 wt.% MWCNTs into cementitious
materials can lead to a 27% decrease in electromagnetic wave
reectivity at a frequency of 2.9 GHz (as shown in Fig. 3c))
[56,66]. Gong et al. studied the effects of CNTs on the dielectric
and piezoelectric properties of PZT cementitious composites. The
 B. Han et al. / Composites: Part A 70 (2015) 6981
(a) Electrical conductivity of CNTs filled cementitious composites [56]
(b) Sensing property of cementitious
composites with CNTs under
compression[100]
Fig. 2. Electrical and sensing properties of typical CNTs/CNFs lled cementitious composites. (For interpretation of the references to color in this gure legend, the reader is
referred to the web version of this article.)
dielectric constant and the dielectric loss increase with CNT con-
tent (as shown in Fig. 4a)), while the piezoelectric strain factor
and the piezoelectric voltage factor both only increase with the
CNT content up to 0.3 vol.%. The highest piezoelectric strain factor
and piezoelectric voltage factor values are 62 pC/N and
60  10 3 Vm/N, which are respectively 41% and 28% higher than
that of the composites without CNTs (as shown in Fig. 4b)) [107].
4.2. NGPs enhanced/modied cementitious composites
Huang et al. observed that the addition of NGPs increases the
exural strength of cementitious composites by 82% compared
with the plain ones. The electrical property of the composites is
signicantly modied, and the composites become highly conduc-
tive (as shown in Fig. 5) [13]. However, compared with Fig. 2a), it is
obvious that the contribution of NGP content to the electrical prop-
erty of the composites is less than that of the same addition of
CNTs. Duan et al. reported that only 0.05% GO can improve the ex-
ural strength of cementitious composites from between 41% to 59%
and the compressive strength from between 15% to 33% [108]. Lv
et al. found that GO nanosheets can remarkably increase the
tensile/exural strength of the corresponding cementitious com-
posites. Especially, when the content of GO is 0.03%, the tensile,
exural and compressive strength of cementitious composites
increases by 78.6%, 60.7% and 38.9%, respectively [109].
Du et al. studied the sensing behavior of NFCC with different
contents of NGPs (04.8 wt.%), and observed that the composites
exhibit a decrease in electrical resistivity and present a good sens-
ing property when NGP content is in the range from 2.4 vol.% to
3.6 vol.% [110]. Singh et al. found that the SET (total SE) of the
GO-ferrouid-cementitious composites is 46 dB, which is much
higher than that of the pristine cementitious composites (4 dB)
73
(c) Sensing property of cementitious composites with
CNFs under bending [22]
[77]. Peyvandi et al. investigated the contributions of NGPs to the
durability of cementitious composites, and observed that NGPs sig-
nicantly improve the moisture transport performance and acid
resistance of the composites at a low dosage (0.05 vol.%) [24].
From these research results, it has been proved that NCMs can
signicantly enhance/modify the mechanical and functional prop-
erties of cementitious composites at a low concentration. However,
the existing researches mainly focus on the enhancement/modi-
cation effects of NCMs on performance parameters of different
cementitious composites. It is necessary to set up some constitu-
tive models for describing and predicting performances of NFCC,
and discover the hidden connections between different perfor-
mances of the composites. In addition, previous researches mainly
investigated the enhancement/modication effect of NCMs to
cementitious composites without coarse aggregate. However, the
cementitious composite with coarse aggregate, i.e. concrete, is
much more useful in real applications. It deserves extensive inves-
tigation on the enhancement/modication of NCMs to concrete.
5. Characterization methods for NFCC
Advances in material characterization techniques and computa-
tional material science have provided us with promising new tools
to better understand and engineer the structure of NFCC and to
enhance/modify properties of cementitious composites.
5.1. Characterization methods of dispersion of NCMs
There are two approaches for characterizing dispersion of
NCMs. One is to observe the solution of NCMs with advanced
instruments such as optical microscopy, scanning electron micro-
scope (SEM), transmission electron microscopy (TEM), Fourier
74 B. Han et al. / Composites: Part A 70 (2015) 6981

(b) Relationships between water absorbing amounts

(a) Representative frequency responses of CNT
and water absorbing time of cementitious materials
enhanced/modified cementitious composites
with and without CNTs (#0 = 0% CNT, #1 = 0.2%
with 0.1% (DMd1), 0.2% (DMd2), 0.5%
CNT + NaDDBS, #2 = 0.2% CNT + SDS. The
(DMd5), 1.0% (DM1) and 2.0% (DM2) of
zoom-out is experimental setup for water sorptivity
CNTs
test. (Q is the volumetric flow rate (m3/s), A is the
cross sectional area perpendicular to the flow
direction (m2)) [15]

(c) Shielding effectiveness (SE) in the frequency range

from 8.2 to 12.4GHz of cementitious composites
with 0, 1, 2, 3, 4, 5, 10 and 15 wt.% of MWCNTs
(OPC, CCNT1-15)[56]

Fig. 3. Other properties of typical CNTs/CNFs lled cementitious composites. (For interpretation of the references to color in this gure legend, the reader is referred to the
web version of this article.)

(a) Dielectric constant and dielectric loss of PZT (b) Piezoelectric strain factor and piezoelectric
cementitious composites with various CNT contents voltage factor of PZT cementitious composites
[107] with various CNT contents [107]

Fig. 4. Dielectric and piezoelectric properties of typical CNTs lled cementitious composites.
 B. Han et al. / Composites: Part A 70 (2015) 6981
Fig. 5. Electrical resistivity of cementitious composites with GNP (i.e. NGPs) [110]
(For interpretation of the references to color in this gure legend, the reader is
referred to the web version of this article.).
transform infrared spectroscopy, Raman spectroscopy, energy dis-
persive X-ray spectrum, environment scanning electron micro-
scope, ultraviolet visible spectroscopy, X-ray photoelectron
spectroscopy, small angle light scattering and atomic force electron
microscopy [11,41,5356,60,75,93]. However, the dispersion of
NCMs in solution cannot fully represent the dispersion of NCMs
in composites. The other one is to observe the distribution of NCMs
in composites through the microanalysis methods, which include
atomic force electron microscopy, SEM, TEM, environment scan-
ning electron microscope, laser ablation inductively coupled
plasma mass spectrometry and so on [35,52,53,55,60,75,93]. In
addition, some researchers tried to employ numerical simulation
methods (3-D simulations and probability density function calcu-
lation) to realize fully determination of the dispersion of NCMs
[78,111].
5.2. Characterization methods of performances of composites
In order to investigate the behaviors in nanoscale of NFCC and
the improvement/modication mechanisms of NCMs to cementi-
tious materials, some advanced instruments including X-ray dif-
fraction, atomic force electron microscopy, mercury intrusion
porosimetry and the accelerated surface area and porosimetry sys-
tem have been used to measure the hydration products, hardness,
Youngs modulus, porosity and pore size distribution of the com-
posites [11,40]. For example, Fig. 6a shows the records of the data
(a) Three-dimensional topographic image of AFM
scanning over CNTs enhanced/modified
cementitious materials [40]
Fig. 6. Test and simulation of properties of typical NFCC. (For interpretation of the references to color in this gure legend, the reader is referred to the web version of this
article.)
75
of load, deection and position with the AFM tip indenting over the
surface of the cementitious composites so that the mechanical
properties of the composites can be measured using the nanoin-
dentation module. In addition, some numerical methods such as
representative elementary volume, numerical analysis, two-
dimensional micromechanical simulations and the nite element
methods, also have been employed to assist in analyzing the com-
pressive strength, tensile strength, cracking strength, bending force
and shear force of NFCC (as shown in Fig. 6b)) [96,112116].
Because the compositions, structures and processing technology
of NFCC are complex in nature, the existing techniques still cannot
realize the full analysis of the properties and microstructures of
NFCC. More advanced tools are needed to help to characterize,
understand and control the structures and properties of NFCC.
6. Enhancement/modication mechanisms of NCMs
6.1. Enhancement/modication mechanisms of CNTs/CNFs
The enhancement/modication of CNTs/CNFs on the properties
of cementitious composites mainly results from the extensive dis-
tribution enhancement network of CNTs/CNFs in composites [56].
Generally, the following factors have contributions to the
mechanical property of composites: (1) Excellent intrinsic proper-
ties of CNTs/CNFs (as shown in Table 1); (2) The nano size effect
and nucleation effect of the CNTs/CNFs including small size effect,
surface effect and high aspect ratio. Makar and Chan observed that
the CNTs appear to act as nucleating sites for the C3S hydration
products (as shown in Fig. 7a)) [117], thus accelerating the hydra-
tion reaction of the C3S (as shown in Fig. 7b)) and increasing the
amount of high stiffness CSH gel (as shown in Fig. 7c)) [52];
(3) Improvement of CNTs/CNFs to microstructures and the interfa-
cial transition zone of composites. For example, the autogenous
shrinkage in composites with CNTs reduces at least 30% after
96 h compared with composites without CNTs (as shown in
Fig. 7d)). Furthermore, the addition of CNTs/CNFs nes pore size
distribution and decreases the porosity (or nanoporosity) of com-
posites by lling the gaps (or pores) between the hydration prod-
ucts such as CSH gel and ettringite. Therefore, the composites
become much more compacted [11,14,52,118,119]; (4) Strong
bonding between CNTs/CNFs and the matrix, especially for the
covalence-modied CNTs/CNFs. For example, Peyvandi et al.
employed hydrophilic groups (COOH) covalence-modied CNFs
to improve interfacial interactions in composites, in which the
COOH groups form strong coordinate bonds with the Ca2+ ions in
(b) Comparison between simulation and
experimental load-deflection response of CNTs
cementitious composites [96]
76 B. Han et al. / Composites: Part A 70 (2015) 6981

Cement sonicated with CNT

Sonicated cement
Cement

(a) TEM images of CNTs (b) Relationship between heat flow and hydration time of cementitious
within the hardened materials (The numbers in Figure identify the peaks as: 1 initial C3A
cementitious composites [44] reactions; 2 C3S surface reactions; 3 the main C3S hydration peak; and 4
ettringite formation) [117]

(d) Comparison of autogenous shrinkage of

(c) Amount of high stiffness C-S-H of cementitious cementitious composites with and without CNTs
composites with CNT [52] [119]

(e) Bonding between modified CNFs with cementitious material [90]

(f) CNF pulled out from a microcrack (g) CNTs embedded in cementitious materials
bridging a crack [44]

Fig. 7. Enhancing effect of CNTs/CNFs to cementitious materials. (For interpretation of the references to color in this gure legend, the reader is referred to the web version of
this article.)

cement hydrates, thus enhancing the mechanical properties of To the conductive and sensing property, the factors that may
composites (as shown in Fig. 7e)) [90]; (5) Crack bridging, pinning make contributions mainly include the intrinsic electrical conduc-
effect, ber pull-out, crack deection, ber debonding and ber tivity, contacting conduction, tunneling conduction and eld emis-
breaking (as shown in Fig. 7(f) and (g)) [14,44]. sion conduction of CNTs/CNFs (as shown in Fig. 8) [14,120122].
 B. Han et al. / Composites: Part A 70 (2015) 6981 77

Fig. 8. Schematic diagram of basic conductive element in conductive network of CNTs cementitious composites [122]. (For interpretation of the references to color in this
gure legend, the reader is referred to the web version of this article.)

Actually, the conduction mechanism of CNTs/CNFs enhanced/mod-
ied cementitious composites is very complex in nature. The
above-mentioned conduction mechanisms coexist in composites
and interrelate each other. One or several factors among these
aspects may be dominant for a specic NFCC. In general, the con-
ductive characteristic of NFCC can be described by the percolation
phenomenon. In addition, the electrical resistivity of NFCC would
change when the composites deform under loading. The factors
that may contribute to the sensing property include (1) the change
of intrinsic resistance of CNTs/CNFs; (2) the change of bonding
between CNTs/CNFs and matrix; (3) the change of contact between
CNTs/CNFs; and (4) the change of tunneling distance between
CNTs/CNFs. It should be noted that the above-mentioned factors
usually work together for the contribution to sensing property of
NFCC, but only one or several of them are leading at certain perco-
lation zones (i.e. content levels of CNTs/CNFs). Therefore, the per-
colation threshold is an important parameter for designing and
optimizing the sensing property of NFCC. Generally, the CNTs/CNFs
concentration above the percolation threshold is benecial for the
sensing sensitivity under tension, while that below the percolation
threshold is benecial for the sensing sensitivity under compres-
sion [14].
The presence of conductive CNTs/CNFs in the insulative cemen-
titious matrix results in space charge accumulating at the inter-
faces, which contributes towards the higher microwave
absorption in the composites [56]. The dielectric constant increases
with the MWCNT content. This improves the capability of the com-
posites to shield electromagnetic waves (as shown in Fig. 9). The
increase in MWCNT leads to a reduction of skin depth and an
increase in AC conductivity along with an improvement of input
impedance. This not only enhances the amount of electromagnetic
radiation penetrating inside the shield but also increases the effec-
tive absorption capability. Therefore, the CNTs/CNFs embedded in
concrete matrix increase the interfacial polarization and the effec-
tive anisotropy energy of composites, thus leading to the high SE of
NFCC [56,66].
The enhancement of CNTs to the piezoelectric and dielectric
properties of PZT cementitious composites can be attributed to
the following reasons, i.e. the CNTs act as conductive llers dis-
persed in the cement matrix, improving the poling efciency of
the PZT cementitious composites and enabling the poling process
to be carried out at room temperature, in contrast to the 120 C
required for the PZT cementitious composites without CNTs [107].
6.2. Enhancement/modication mechanisms of NGPs
As a type of nano-particles with two-dimensional structure,
NGPs possess the small size effect that enables NGPs to serve
as nuclei. For example, GO nanosheets could regulate formation
of ower-like crystals (as shown in Fig. 10). The formed network
structure of cement hydration products around the NGPs can
improve the homogeneity and compactness of the hardened
cementitious composites. For example, additions of 0.05% GO
decrease the total porosity of cementitious composites from
32.6% to 28.2% (as shown in Fig.11). NGPs also have the surface
effect, which leads to enormous interface areas. At the interfaces,
NGPs possess an intimate bonding with the cement matrix due to
strong Van der Waals forces. The large aspect ratio and plate shape
of NGPs give themselves strong abilities to block and divert the
micro cracks, which can slow down crack propagation and forma-
tion of the crack network. The bridge effect of NGPs can delay crack
origination and prevent crack opening up. In addition, NGPs also

(a) variation of dielectric constant (b) dielectric loss

Fig. 9. Behavior of dielectric constant of MWCNT enhanced/modied cementitious composites with 0, 1, 2, 3, 4, 5, 10 and 15 wt.% of MWCNTs (OPC, CCNT1-15)[56]. (For
interpretation of the references to color in this gure legend, the reader is referred to the web version of this article.)
78 B. Han et al. / Composites: Part A 70 (2015) 6981
Fig. 10. Schematic diagram of regulation mechanism of GO on cement hydration crystals [109].
Fig. 11. Pore size and distribution of GO enhanced/modied cementitious com-
posites [108]. (For interpretation of the references to color in this gure legend, the
reader is referred to the web version of this article.)
can enhance mechanical properties of these composites via the
crack-arresting effect and the improvement to the interfacial tran-
sition zone of NFCC [13].
For the electrical property of NFCC, Huang proposed several the-
ories on the mechanism of the contributions of NGPs to cementi-
tious materials based on the characteristics of NGPs. NGPs have
the pi-electrons that participate in interlayer pi bonding. This
makes NGPs become a good electrically conductive material. In
addition, the carbonation process with temperature up to
1050 C during fabrication of NGPs leaves a large excess of holes
in the valence band. Due to this characteristic of NGPs, they con-
tribute to the electrical property of NFCC through the following
paths: (1) Electronic conduction and hole conduction through
NGPs by the tunneling effect; (2) Electronic conduction and hole
conduction through contacting conduction of NGPs [13]. The two
factors both contribute to the electrical property of NFCC, but
one of them may be dominant for certain content of NGPs.
The action mechanism of NGPs on the EMI property of NGPs
enhanced/modied cementitious composites is similar to that of
CNFs/CNTs enhanced/modied cementitious composites [77].
Overall, the above researchers observed some evidences to
explain the enhancement/modication mechanism of NCMs to
cementitious composites. However, these evidences just provided
qualitative or descriptive explanations, because their contributions
to performances of the composites are complex in nature. There-
fore, it is necessary to try to build up useful quantitative correla-
tions between the components, processing or microstructures
and the properties of NFCC.
7. Structural applications
The current applications of NFCC mainly focus on two aspects.
One aspect is to enhance mechanical performances and durability
of structures or structural components (e.g. concrete beams, col-
umns and pipes). For example, Hunashyal et al. investigated the
behavior of beams fabricated with MWCNTs enhanced/modied
cementitious composites [58]. The exural strength of the beam
is increased by 43.75% at MWCNT addition of 0.75 wt.%. Gao
et al. employed CNFs in cylinders to enhance the mechanical prop-
erties. The peak compressive strength of the cylinders increases by
21.4% when the CNF concentration is 1%. Moreover, the stiffness of
the cylinders containing CNFs is much higher than that of the plain
ones [95]. Peyvandi et al. added the modied NGPs into the dry-
cast concrete pipes in aggressive sanitary sewer environment to
improve their durability characteristics including the moisture
sorptivity and acid resistance, thus increasing their service life in
sanitary sewer applications [24].
The other one aspect is to use their functional performances for
structural health monitoring or trafc detection [123]. For exam-
ple, Howser et al. built shear-critical columns with cementitious
composites containing CNFs. The columns are capable of strain
 B. Han et al. / Composites: Part A 70 (2015) 6981
self-sensing under a reversed cyclic load and damage self-assess-
ment [73]. Saa embedded cementitious composites with SWCNTs
into the tensile region of beams to set up the self-sensing struc-
tures subjected to monotonic and cyclic bending. The self-sensing
structures can detect crack propagation and damage accumulation
during loading [124]. Baeza et al. embedded and bonded cement-
itous composites with CNFs into different service locations of rein-
forced beam [22]. The composites with CNFs can achieve elastic
strain sensing of compression and tension region of beam and
capable of measuring strains on the surface of a structural element
[14,73,124,125]. Han et al. developed self-sensing pavements with
cementitious composites containing CNTs and investigated the fea-
sibility of using the self-sensing pavements for trafc monitoring
with vehicular loading experiments. The proposed self-sensing
pavement system can accurately detect the passing of different
vehicles under different vehicular speeds and test environments
[14,61,100,101,126].
Up to now, the researches on the NFCC still focus on their fab-
rication and properties. A few investigations are performed on
the structural application of these composites. However, the NFCC
exhibit excellent structural and functional performances, which is
very benecial for the synthesis performances of components or
structures fabricated with them. The mechanical, durable and
functional properties and the design methods of the components
and structures both deserve extensive investigation to promote
engineering application of these composites.
8. Conclusions
Ultra miniature tiny nano materials bring tremendous change
to the world including the eld of construction, expanding the hor-
izontal of research in multifunctional cementitious composites.
Their extraordinary physical properties, size effect, and chemical
and thermal stability are benecial for enhancing/modifying the
mechanical, electrical, thermal, electromagnetic shielding and
durable properties of cementitious materials.
Although a great deal of research has been conducted in this
area over the past decade, there still exist a lot of challenges
needed to be addressed. Future work on NFCC may include the
investigations of the simple, repeatable, large-scale and low-
energy consumption methods for dispersing NCMs in cementitious
composites, the enhancement/modication effect of NCMs to con-
crete with coarse aggregate, other structural and functional prop-
erties of NFCC such as durability, thermoelectric and the precise
explanation of the enhancement/modication mechanisms of
NCMs to composites by numerical simulation or new characteriza-
tion methods, the constitutive models of performances of NFCC,
the performances and their constitutive models of the structures
made with NFCC, etc.
NFCC can help to develop infrastructures with elegantly inte-
grated excellent structural performances, high durability and mul-
tifunctional/smart capability, thus improving safety, serviceability,
reliability and durability of infrastructures. As a new generation of
construction materials, they will promote sustainable develop-
ments in the eld of concrete materials and structures.
Acknowledgments
The authors thank the funding supported from the National
Science Foundation of China (51178148, 51428801), the Program
for New Century Excellent Talents in University of China
(NCET-11-0798), and the Ministry of Science and Technology of
China (2011BAK02B01).
79
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Further reading
[89] Nasibulina LI, Anoshkin IV, Nasibulin AG, et al. Effect of carbon nanotube
aqueous dispersion quality on mechanical properties of cement composite. J
Nanomater 2012;169262:6.