sensors

Review
Cement-Based Piezoelectric Ceramic Composites for Sensing
Elements: A Comprehensive State-of-the-Art Review
Weijian Ding 1,2 , Yuqing Liu 1,3, * , Tomoki Shiotani 1 , Quan Wang 2 , Ningxu Han 3 and Feng Xing 3

1 Department of Civil and Earth Resources Engineering, Graduate School of Engineering, Kyoto University,
Kyoto 615-8540, Japan; [email protected] (W.D.); [email protected] (T.S.)
2 Department of Mechanics and Aerospace Engineering, Southern University of Science and Technology,
Shenzhen 518055, China; [email protected]
3 Guangdong Province Key Laboratory of Durability for Marine Civil Engineering, College of Civil and
Transportation Engineering, Shenzhen University, Shenzhen 518060, China; [email protected] (N.H.);
[email protected] (F.X.)
* Correspondence: [email protected]; Tel.: +81-075-383-3496

Abstract: Compatibility, a critical issue between sensing material and host structure, significantly
influences the detecting performance (e.g., sensitive, signal-to-noise ratio) of the embedded sensor.
To address this issue in concrete-based infrastructural health monitoring, cement-based piezoelectric
composites (piezoelectric ceramic particles as a function phase and cementitious materials as a
matrix) have attracted continuous attention in the past two decades, dramatically exhibiting superior
durability, sensitivity, and compatibility. This review paper performs a synthetical overview of recent
advances in theoretical analysis, characterization and simulation, materials selection, the fabrication



process, and application of the cement-based piezoelectric composites. The critical issues of each


part are also presented. The influencing factors of the materials and fabrication process on the final
Citation: Ding, W.; Liu, Y.; Shiotani,
performance of composites are further discussed. Meanwhile, the application of the composite as a
T.; Wang, Q.; Han, N.; Xing, F.
sensing element for various monitoring techniques is summarized. Further study on the experiment
Cement-Based Piezoelectric Ceramic
and simulation, materials, fabrication technique, and application are also pointed out purposefully.
Composites for Sensing Elements: A
Comprehensive State-of-the-Art
Review. Sensors 2021, 21, 3230.
Keywords: sensing element; piezoelectric ceramic composite; fabrication; properties; structural
https://doi.org/10.3390/s21093230 health monitoring

Academic Editor: Theodore

E. Matikas
1. Introduction
Received: 8 April 2021 Infrastructure, a series of fundamental facilities and structure systems, performs
Accepted: 5 May 2021
indispensable support for society, expected to achieve sustainability and economic effi-
Published: 7 May 2021
ciency. However, safety hazards caused by progressive deterioration with age [1] and
serious disasters related to severe environmental conditions (freeze–thaw cycles [2,3],
Publisher’s Note: MDPI stays neutral
marine environment [4], high temperature [5], etc.) are the potential issues during the
with regard to jurisdictional claims in
lifespan of infrastructure, possibly leading to a shortened service life and high mainte-
published maps and institutional affil-
nance/reconstruction costs. Concrete, regarded as an affordable, durable, and dramatic
iations.
building material, has been widely applied in infrastructure [6–10]. Due to the adverse im-
pact of intrinsic (material self-defects [11], deficient structural design and construction, etc.)
and extrinsic (severe environment, accidental loading [12], etc.) factors, concrete structures
usually undergo deterioration during the whole lifespan, such as concrete cracking [13],
Copyright: © 2021 by the authors.
steel corrosion [14,15], spalling [16], and structure collapse [17].
Licensee MDPI, Basel, Switzerland.
Most serious durability and safety issues for concrete-based infrastructure are usually
This article is an open access article
the cumulative consequence induced by the service environment [18,19], aging [20], and
distributed under the terms and
self-defects [21]. At different periods of its lifespan, there are various dominant factors
conditions of the Creative Commons
for degeneration. In the concreting process, fresh concrete can be easily influenced by
Attribution (CC BY) license (https://
temperature, humidity, and rheological properties, possibly leading to self-defects (cracks
creativecommons.org/licenses/by/
4.0/).
and pores). During the service life, aggressive action related to the invasive substances

Sensors 2021, 21, 3230. https://doi.org/10.3390/s21093230 https://www.mdpi.com/journal/sensors

Sensors 2021, 21, 3230 2 of 29

(chloride, carbon dioxide, and sulfate, etc.) and environmental change is the major reason
for the deterioration (e.g., corrosion, carbonation, and cracking). As concrete structures
age, the deterioration will decrease the ultimate load capacity and further bring safety and
serviceability risks. The application of eco-friendly materials (e.g., recycled concrete [22]
and aggregate [10], seawater [23] and sea sand [24], and geopolymer [25,26]) in construc-
tion is another challenge for the structural performance. Due to durability and safety
issues, concrete-based infrastructure will struggle to maintain functionality, and the most
affordable solution (e.g., repair, upgrade, and partial reconstruction) needs to be filtrated.
Considering the severe consequences caused by structural deterioration, there is a
strong demand for implementing identification strategies and protection for concrete-based
infrastructure. An innovative, reliable, and cost-effective structural health monitoring
(SHM) technique for constructing/existing infrastructure has been an essential item to
diagnose and mitigate damages and further ensure its functionality, thereby elongating the
service life. The strategy of efficient and accurate SHM systems with intelligent materials
(e.g., optical fiber [27], piezoelectric materials [28]) installed in concrete structures has
attracted lots of attention in recent decades [29–32]. Piezoelectric materials can be encapsu-
lated as smart aggregates and embedded into the concrete structure, thereby monitoring
the deterioration process. The distinction in acoustic impedance, density, and mechanics
properties leads to the lower compatibility between the sensing element and host structures,
resulting in signal capture disturbance. Table 1 summarizes the major parameters that
lead to the incompatibility among cement, concrete and piezoelectric ceramics. One of the
critical factors for signal acquisition is acoustic impedance, determined by the density and
acoustic velocity [33]. The acoustic velocities of piezoelectric ceramic, cement, and plain
concrete are similar, while the density of piezoelectric ceramic is much higher, resulting in
the acoustic impedance mismatching problem. The piezoelectric composite is an alternative
approach to address this issue. In 2002, cement-based piezoelectric composites (CPCs),
innovated by Li et al. [34], are regarded as a pioneering inorganic piezoelectric composite,
more adaptable to the concrete structure. Based on the connectivity, piezoelectric composite
materials can be divided into 10 basic types [35]. The superiority of the 0-3/1-3/2-2 type
CPCs applied in SHM has been demonstrated. The 1-3 [36]/2-2 [37] types can be regarded
as the development based on 0-3 by controlling the distribution of piezoelectric materials
in the cement matrix. Despite the lower piezoelectric strain constant (d33 ), 0-3 CPCs show
an excellent overall performance (e.g., higher piezoelectric voltage constant (g33 ), acoustic
impedance matching, and flexibility) as a better alternative material for sensing elements,
and also show a prospect in combining intelligent manufacturing. However, the difference
in fabrication parameters and various raw materials sources leads to a great variety in the
final piezoelectric performance.

Table 1. Physical properties of piezoelectric ceramic, cement paste and concrete.

Materials
Items
Piezoelectric Ceramic Cement Paste Plain Concrete
Density (103 kg/m3 ) 4.64–7.6 [33,38,39] 2.0–2.2 [37] 2.4 [40]
Acoustic velocity (103 m/s) 2.83–3.40 [40] 2.64–3.37 [37,40] 3.0–4.2 [37,40]
Acoustic impedance (MRayl) 21.2–30 [37] 3.5–8 [41] 6.9–10.4 [42]
Elasticity modulus (GPa) 50–75 [38,43] 10–20 [44] 19.0–48.6 [45]

In the last two decades, the performance improvement of CPCs has been performed.
The significant variety in the final piezoelectric performance illustrates the existing short-
coming and insufficient understanding around the composite. Our main objective in this
review is to recapitulate the previous studies related to CPCs and discuss the influence of
raw materials and the main problems in fabrication, thereby promoting advanced piezo-
electric composite design, fabrication, and application. Moreover, the present review will
summarize previous research to sort out the critical influencing factors and potential di-
Sensors 2021, 21, 3230 3 of 29

rections. Then, to clarify the influencing factors of the composite materials, theories and
fundamentals, experimental and modeling analysis, raw materials, the fabrication process,
and application are presented in different sections. At the end of each section, insightful
viewpoints and prospective studies on the composite will be provided.

2. Recent Study on Cement-Based Piezoelectric Composites

The piezoelectric performance (e.g., piezoelectric, electromechanical coupling, and
dielectric properties) of CPCs has been comprehensively characterized and discussed.
Initially, Li et al. [30] reported the feasibility of CPCs and characterized their perfor-
mance, including the piezoelectric strain factor (d33 ), piezoelectric voltage factor (g33 ),
electromechanical coupling coefficient (Kt and Kp ), and dielectric constant (εr ). Subse-
quently, Huang et al. [46] studied the polarization process of PZT/sulphoaluminate cement
composites; Chaipanich et al. [47] demonstrated the properties of PZT–ordinary Portland
cement composites. These studies have demonstrated the feasibility of CPCs and revealed
that the piezoelectric particles’ higher content could improve the piezoelectric performance.
Additionally, Chaipanich et al. [48] studied the particle size effect, showing that a larger
particle of the function phase is beneficial for improving the d33 and εr . Pan et al. [49] and
Chomyen et al. [50] demonstrated improved piezoelectric performance by adding fly ash,
respectively. However, the final piezoelectric performance shows a tremendous difference,
mainly attributed to the difference in piezoelectric materials and polarization parameters.
According to the above researches, the main influencing factors on the all-round perfor-
mance can be summarized as the (a) matrix; (b) functional phase (piezoelectric materials);
(c) fabrication process; (d) aging.
Due to the complex hydration product composition and heterogeneous microstruc-
ture, the matrix effect on piezoelectric performance has been investigated. Among these,
enhancing d33 is still the primary target. The low-efficiency stress transfer between ma-
trix and piezoelectric particles caused by the poor connectivity and porosity is the main
reason for the lower d33 . Therefore, a denser matrix is a penitential approach to optimize
it. Chaipanich et al. [51] revealed that the d33 shows a slight increase with adding silica
fume. Wang et al. [52] found that adding silica-based material can improve the d33 even up
to 99.0 pC/N due to the ITZ optimization under the conditions of compression forming,
steam curing, and aging. Subsequently, to decrease porosities, slag, fly ash, and kaolin was
studied by Pan et al. [49,53], tracing the piezoelectric properties in different ages, and the
highest d33 can reach 111.1 pC/N. Wittinanon et al. [38] employed PVDF to modify the ITZ
and reduce the porosity, showing a significant optimization in reducing leakage current.
Considering the positive effect of the higher matrix conductivity during the polarization
process, carbon materials (carbon addition [54], carbon black [55,56], carbon nanotube [57],
and graphene nanoplatelets [58]) were also applied to optimize the piezoelectric properties.
The matrix properties can also affect the g33 , Kt , Kp , εr , and dielectric loss (tan δ), and
the increase of parameter values (Kt , εr , and g33 ) with the help of admixture has been
reported [49,55]. The output voltage (V) of the composite mixed with basalt fiber, which
affects the matrix’s elastic modulus, was also characterized [43].
Meanwhile, the fabrication process optimization was also carried out, and some steps
demonstrate significant improvement. Huang et al. [59] applied the forming pressure
to fabricate the CPCs, which could help obtain a denser matrix and further enhance the
d33 . Furthermore, the curing is also essential to obtain the higher piezoelectric perfor-
mance because inadequate curing would cause interfacial cracks and lead to a locally poor
value of d33 . Considering the positive effect of the high temperature on the hydration
evaluation, Wang et al. [52] carried out the hot water and steam curing process, respec-
tively. Pan et al. [60] found that the pre-heating treatment could improve the polarization
efficiency due to decreased moisture. The above fabrication process development could
contribute to a better microstructure and mitigate the negative effect caused by the ITZ
between the cement matrix and piezoelectric ceramic particles. The significance of polar-
Sensors 2021, 21, 3230 4 of 29

ization has been studied by Huang et al. [46] and Dong et al. [61], demonstrating that the
voltage, polarization time, and temperature can directly play a decisive role.
Recently, the multi-factors coupling for the design and fabrication of the composite
has been considered. Among those factors, aging is the key influential factor combined
with the materials and fabrication process for the performance of CPCs. Dong et al. [37] and
Huang et al. [62] revealed the d33 increase with time, even though the matrix phase in their
studies is different. Later, Chaipanich et al. [63] found the increased trend of d33 in PZT-
Portland cement composites with time; Pan et al. [53] also characterized this phenomenon
during their investigation into the effect of admixture. In 2016, Pan et al. [60] found that
heat treatment could improve the comprehensive performance after aging. Subsequently,
the effect of the water/cement ratio and time on the piezoelectric performance was also
studied [64].
The application of this composite has been carried out. Lu et al. [29,30,40,65] systemi-
cally monitored the different states in concrete using embedded CPCs sensors, including
hydration, crack, and corrosion. Xing et al. [66] tested the electrical response of this material
under different mechanical loadings. Pan et al. [31] applied the composite for monitoring
the strength growth of concrete via electromechanical impedance. Those applications
reveal the feasibility and superiority of CPCs as a potential sensing element.
Regarding the environmental issues, lead-free piezoelectric material has attracted
increasing attention. Rianyoi et al. [38,67–69] prepared the barium titanate-cement compos-
ites and characterized the influence of the particle size and polyvinylidene fluoride (PVDF).
Chaipanich et al. [39,50,70–73] fabricated barium zirconate titanate-cement composites
and studied their microstructure and piezoelectric performance. Hunpratub et al. [74]
believe that BCTZO (Ba0.85 Ca0.15 Ti0.9 Zr0.1 O3 ) particle is an alternative material as function
phase and revealed the effect of particle size on dielectric and piezoelectric properties.
Additionally, BNBT (0.94(Bi0.5 Na0.5 )TiO3 -0.06BaTiO3 ) [75] and BNBK (0.88Bi0.5 Na0.5 TiO3 -
0.08Bi0.5 K0.5 TiO3 -0.04BaTiO3 ) [76] have been used as a function phase to fabricate the
composite. Although lead-free piezoelectric materials are potential functional materials,
the lower piezoelectric properties and poor temperature stability still limit their application
in CPCs.
Numerous studies have illustrated the feasibility to fabricate and employ this compos-
ite as a sensing element. However, the effect of the fabrication process and polarization
parameters are still essential to further study due to the physical and chemical distinc-
tion between cementitious materials and piezoelectric materials. The properties of lead-
based/lead-free piezoelectric ceramic and its cement-based composites in recent studies,
including d33 , g33 , εr , Kt , and acoustic impedance, are intuitively summarized in Table 2.
The highest value of d33 in lead-free CPCs is 61.5 pC/N, while that of lead-bearing CPCs is
87 pC/N initially. However, the d33 of the lead-bearing composite can reach over 140 pC/N
after aging, close to the piezoelectric ceramic. It should be mentioned that these higher
parameters almost attribute to the positive effect of aging, and the typical studies for tracing
the change of d33 with aging are illustrated in Figure 1. Only a few studies can obtain high
piezoelectric performance at the initial stage after polarization. Santos et al. [77] reported
that the curing process of CPCs has a direct relationship with its dielectric properties and
electrical conductivity, attributing to the existence of unstable dipoles, which would be a
suitable example for understanding the performance variation, illustrating the significant
effect of the matrix properties on the final performance. Kantakam et al. [78] revealed the
tremendous influence of the matrix material on the dielectric properties.
Sensors 2021, 21, x FOR PEER REVIEW 5 of 31

Table 2. Piezoelectric properties of piezoelectric materials.

Sensors 2021, 21, 3230 5 of 29
Piezoelectric Materials
Items Lead-Based Piezoelectric Lead-Free Lead-Bearing Lead-Free
Ceramic Piezoelectric Ceramic CPCs CPCs
Piezoelectric strain factor d33 Table 2. Piezoelectric properties of piezoelectric materials. 0.5~87 [45,80] 4~61.5
215~513 [79] 190~235 [38,39]
(10 C/N)
−12
Piezoelectric Materials 5 *~143 * [37,52,64] [74,75]
Items
Piezoelectric voltage factor g33 Lead-Based Lead-Free 15~60 [34,81,82] 7~33.59
Lead-Bearing CPCs Lead-Free CPCs
15.9~25
Piezoelectric [79] Piezoelectric
Ceramic 12.43~18.28
Ceramic [38,39]
−3
(10 strain
Vm/N) 20 *~30 * [83] [38,75]
Piezoelectric factor d33 0.5~87 [45,80]
− 12 215~513 [79] 190~235 [38,39] 5 *~143 *43.5~536 4~61.5 [74,75]
[37,52,64][34,47,48]
(10
Dielectric C/N)
constant εr
Piezoelectric voltage factor g33 120~350
1050~3643
15.9~25 [79] [37,77] 12.43~18.28
1452~1726 15~60 [34,81,82]
[38,39] [38,39] 1017.6~1834.2 [78] 7~33.59[38,39]
[38,75]
(10−(at 1 kHz)
3 Vm/N) 20 *~30 * [83]
280 *~890 * [60,64]
43.5~536 [34,47,48]
Dielectric constant εr 1050~3643 [37,77] 1452~1726 [38,39] 9.47~28.19
1017.6~1834.2 [78] [34,79]120~350 [38,39]
(atelectromechanical
Thickness 1 kHz) 280 *~890 * [60,64]
Thickness
40~67 [79] - 13.16 *~13.53 * 9~14 [67]
couplingelectromechanical
coefficient Kt (%) 40~67 [79] - 9.47~28.19 [34,79] 9~14 [67]
coupling coefficient Kt (%) [53,60]
13.16 *~13.53 * [53,60]
Acoustic
Acoustic impedance
impedance 7.5~10.5
21.2~36 [33,37] 25.2~34 [33,38] ~9.6 [32]
Z (106 kg/m 2 s) 21.2~36 [33,37] 25.2~34 [33,38] ~9.6 [32] 7.5~10.5 [67,70,75]
Z (10 kg/m s)
6 2 [67,70,75]
* Range of maximal value after aging in references.
* Range of maximal value after aging in references.

(a) (b)
Figure 1. (a) Piezoelectric strain constant of cement piezoelectric composites.
composites [83]; (b) Piezoelectric
Reprinted strain factor
with permission of 70%
from ref. [83].
PZT/cement composites versus age [64].
Copyright 2016 Elsevier. (b) Piezoelectric strain factor of 70% PZT/cement composites versus age. Reprinted with
permission from ref. [64]. Copyright 2013 Elsevier.
3. Theory, Experiment and Simulation
3. Theory,
3.1. Experiment
Fundamentals and Simulation
of Cement-Based Piezoelectric Composites
3.1. Fundamentals of Cement-Based
Rigorous theoretical analysisPiezoelectric
can describe Composites
the approach to achieve acoustic imped-
ance matching, aiming to reduce signal reflection approach
Rigorous theoretical analysis can describe the and loss. to
For the concrete-based
achieve struc-
acoustic impedance
matching,
tural healthaiming to reduce
monitoring, theresignal reflection andinterface
is a non-negligible loss. Forbetween
the concrete-based structural
the host structure and
health monitoring,
sensor there is
during the elastic a non-negligible
wave propagationinterface between
process [33]. The the host structure
interface will leadand sensor
to partial
duringenergy
signal the elastic
loss.wave propagation
The CPCs have beenprocess [33]. The
developed interface
to reduce will
the lead toinfluence
interface partial signal
and
energyhigh-quality
obtain loss. The CPCs haveThe
signals. been developed
basic to reduce
properties of hostthe interface
materials influence
and and obtain
piezoelectric com-
high-quality
posite signals.
are needed The basic properties
to accomplish of host matching,
the impedance materials and piezoelectric
including composite
the density, are
volume
needed to accomplish the impedance matching, including the density, volume
percentages, and elastic moduli. Subsequently, the density and elastic moduli of compo- percentages,
and elastic
sites moduli. Subsequently,
can be calculated by Equations the density
(1) and and elastic moduli
(2), respectively [34]: of composites can be
calculated by Equations (1) and (2), respectively [34]:
𝜌 =𝜌 𝑣 +𝜌 𝑣 (1)
ρ c = ρ1 v1 + ρ2 v2 (1)

1
Ec = , (2)
v1 /E1 + v2 /E2
Sensors 2021, 21, 3230 6 of 29

where ρ and E represent the density and elastic moduli, respectively; subscript c, 1, and 2
stands for the composite, ceramic particle, and cement matrix, respectively; ν represents
the volume percentage.
Then, the acoustic velocity (Vc ) and acoustic impedance (Zc ) of CPCs can be expressed
as Equations (3) and (4), respectively.
 1/2
Ec
Vc = , (3)
ρc

Zc = ρc Vc = (ρc Ec ) /2 ,
1
(4)
Thus, the acoustic impedance of CPCs can be adjusted based on Equation (4), thereby
achieving acoustic impedance matching.
In terms of function, the piezoelectric effect is the source of the mechanical–electrical
conversion of piezoelectric materials related to the asymmetric crystal structure. It can
be divided into direct and reverse piezoelectric effects. The direct piezoelectric effect,
an essential basis of the piezoelectric sensor, describes the free electric charges on the
crystal surface induced by mechanical force; the reverse piezoelectric effect refers to the
mechanical deformation of the crystal caused by the external electric field, also known as
the electrostrictive effect. Since discovering the piezoelectric effect in quartz crystals in the
1980s, the fundamentals for piezoelectric materials have been deeply studied.
The stress (T) and electric field (E) can both directly induce electric displacement (D)
for piezoelectric materials. The D directly aroused by the T is [84]:

D = dT, (5)

where d present the piezoelectric strain constant. Under the internal electric field (E)
without external stress, D can be given by:

D = ε T E, (6)

where εT presents the dielectric permittivity for constant stress. Moreover, the strain of the
piezoelectric materials can be caused by T and internal E, respectively.

S = sE T, (7)

S = dE, (8)
where sE is the elastic compliance for the constant electric field.
Furthermore, the coupling between dielectric and elastic properties of the piezoelectric
materials can be described by a linear relationship between two electrical (E and D) and
mechanical (T and S) variables, illustrating the direct and reverse piezoelectric effects, and
the state equations are:
D = dT + εT E, (9)
S = sE T + dE, (10)
when S and E are selected as variables, the state equation of the piezoelectric effect can be
written as [66]:
T = cE S − em E, (11)
D = en S + εS E, (12)
where cE represents the elastic stiffness coefficient with a constant electrical field; em and en
represent the piezoelectric stress coefficient, respectively; εS denotes the dielectric coefficient
with constant strain. Equations (11) and (12) are regarded as more convenient equations to
describe the piezoelectric effect of ferroelectric crystal, which have been applied to study
CPCs under the mechanical loadings condition [66].
Sensors 2021, 21, 3230 7 of 29

A clear description of the mechanical–electrical conversion relationship between the

matrix and piezoelectric particles is vital in the piezoelectric composite. For the CPCs, the
external stress is acting on the non-piezoelectric matrix instead of piezoelectric particles,
and the direct piezoelectric effect is relative to the volume percentage of piezoelectric
materials. A two-phase system (as depicted in Figure 2) which has been employed to
describe the epoxy/PZT composite systems, can be used to describe the piezoelectric effect
of cement/PZT composites. Based on the elastic constant (c1 and c2 ) and dielectric constant
(ε 1 and ε 2 ) of two phases and the volume percentage of Phase 2(∅), the apparent elastic
constant c and dielectric constant ε of the two-phase system are shown as below:

3(1 − ∅)c1 + (2 + 3∅)c2

c= c , (13)
(3 + 2∅)c1 + 2(1 − ∅)c2 1

2(1 − ∅)ε 1 + (1 + 2∅)ε 2

ε= ε , (14)
(2 + ∅)ε 1 + (1 − ∅)ε 2 1
These two constants can help to understand the relationship between electric dis-
placement and strain. Figure 3 elucidates the piezoelectric effect of the two-phase system,
different from that of piezoelectric ceramics. The direct piezoelectric effect can be written as:

D = eS, (15)

However, Phase 1 is the non-piezoelectric matrix without the piezoelectric effect. The
only approach to induce the direct piezoelectric effect is applying stress to Phase 2, the
piezoelectric spherical phase. To elucidate the direct piezoelectric effect, a piezoelectric
constant e is defined:    
D T
e= =− , (16)
S E E s
The strain acting on the two-phase system will produce the local strain in Phase 2 due
to the strain induced by external loading in Phase 1.

S2 = Ls S, (17)

where S2 is the local strain in Phase 2, Ls is the local field coefficients with respect to
strain (S).
Subsequently, the local electric displacement (D2 ) is aroused by S2 .

D2 = e2 S2 , (18)

where e2 represents the piezoelectric constant of Phase 2, and the relationship between e
and e2 can be expressed as:
e = ∅ L s L E e2 , (19)
where Ls and L E represent the local field coefficients with reference to S and E, respectively.
In the condition of E = 0, the apparent electric displacement D aroused by D2 can be
written as:
D = ∅ L E D2 , (20)
The local field coefficients Ls and L E are calculated based on Equations (13) and
(14) [85–88]:
5c1
Ls = , (21)
(3 + 2∅)c1 + 2(1 − ∅)c2
3ε 1
LE = , (22)
(2 + ∅)ε 1 + (1 − ∅)ε 2
 𝑣 1
𝑑 =𝑑 ∙ ⁄ ⁄ 𝜀 ∙ ⁄
, 𝑐𝑢𝑏𝑒 𝑚𝑜𝑑𝑒𝑙 (28)
𝑣 + 1−𝑣 ∙ 1−𝑣 +𝑣
𝜀

Sensors 2021, 21, 3230 where 𝑑 , 𝑣, and 𝑆 represent the piezoelectric strain factor, volume percentage,8 of
and29
elastic compliance, respectively; super-/subscript 1 and 2 stand for the cement matrix
phase and ceramic phase, respectively.

Figure 2.
Figure 2. Two-phase
Two-phasesystem
systemcomposed
composedofofa anon-piezoelectric
non-piezoelectriccontinuous phase
continuous (Phase
phase 1) and
(Phase a a
1) and
piezoelectric spherical
Sensors 2021, 21, x FOR PEER REVIEW
piezoelectric spherical phase
phase (Phase
(Phase 2)
2).[87]. 9 1973
Reprinted with permission from ref. [87]. Copyright of 31

John Wiley & Sons, Inc.

Figure 3. Piezoelectric
Piezoelectriceffect
effectfor
fora a
two-phase system
two-phase [87].Reprinted with permission from ref. [87].
system.
Copyright 1973 John Wiley & Sons, Inc.
3.2. Performance and Microstructure Characterization
Therefore, the local strain and field coefficients are the major factors affecting the
As an alternative functional material for sensing elements, it is essential to character-
piezoelectric performance, which relate to the dielectric constant of two phases and the
ize the piezoelectric performance. The piezoelectric strain factor (d33) and piezoelectric
volume percentage.
voltage factor (g33) of CPCs related to the macroscopic physical quantity are the basic pa-
To predict the piezoelectric properties of the composite, the cube, parallel and series
rameters, which characterize the coupling relationship between the elastic and electrical
theoretical models have been employed [34,69,88]. The results [34,61,69,88,89] reveal that
polarization effects of piezoelectric bulk. Dielectric constant (εr) and dielectric loss (tan δ)
the cube model is more suitable for piezoelectric properties prediction of 0-3 cement-based
are the other factors to evaluate the convenience of polarization. The impedance spectrum
piezoelectric ceramic composite. For the dielectric constant, the theoretical predictions
is used to obtain electromechanical coupling coefficients (Kt and Kp) and further charac-
according to different models are calculated as follows [69,88]:
terize the mechanical–electrical conversion efficiency of the piezoelectric composites. The
mechanical quality factor (Qm1), describing v1 v2 the ability to overcome the energy consumed
=
by internal friction in the piezoelectric + , (seriesstate, is)another critical parameter.(23)
model
ε ε 1 resonance
ε2 Re-
cently, lead-free piezoelectric materials have been employed as function phases in CPCs,
such as BT, BZT, and BCTZO. ε 1 ·v1 + ε 2 ·vet
ε =Chaipanich 2 , al.
(parallel
[68,71]model )
employed (24)
the polarization-electric
ε 1 ·ε 2
field loops (P-E loops) to characterize the ferroelectric hysteresis
  properties of BT/BZT ce-
ε= + ε 2 · 1 − v2/3
1 , (cube model) (25)
ment composites.(ε 2 − ε 1 )·v−1/3 + ε 1 ·v−2/3
1 1
Considering the coupling complexity between the cement matrix and ceramics par-
The theoretical models for piezoelectric strain factor are [89,90]:
ticles, a microstructural analysis of the composites was conducted to evaluate the optimi-
zation process. Jaitanong et al. [91] employed piezo-response force microscopy to investi-
v1 ·d133 ·ε 2 + v2 ·d233 ·ε 1
gate the microstructured33 of=
the composite , (seriesthereby
after hydration, model) characterizing the local
(26)
ε · v1 + ε 1 · v2
piezoelectricity of the domains of 2PZT particles. Potong et al. [72] considered the effect of
the complex hydration conditionv1 ·d133 ·and2 +
S33 the
v2 ·various
d233 ·S331 hydration products in the cementitious
material and applied 33d =
linear voltage-differential
2 · v + S1 · v
, (parallel model
transformer )
dilatometer (27)
to test the ther-
S33 1 33 2
mal expansion, indicating that the thermal expansion the coefficient of the composites
with 30~70% BZT ceramic powder is similar to that of concrete. Wittinanon et al. [39] eval-
uated the effect of PVDF on the composite’s mechanical properties using the indentation
technique. Moreover, acoustic impedance, porosity, and leakage current of the composite
with different PVDF content were also characterized [38].
Sensors 2021, 21, 3230 9 of 29

v2 1
d33 = d233 ·   · , (cube model) (28)
v1/3
2 + 1 − v1/3
2 · ε2 1 − v1/3
2 + v2
ε1

where d33 , v, and S33 represent the piezoelectric strain factor, volume percentage, and
elastic compliance, respectively; super-/subscript 1 and 2 stand for the cement matrix
phase and ceramic phase, respectively.

3.2. Performance and Microstructure Characterization

As an alternative functional material for sensing elements, it is essential to characterize
the piezoelectric performance. The piezoelectric strain factor (d33 ) and piezoelectric voltage
factor (g33 ) of CPCs related to the macroscopic physical quantity are the basic parameters,
which characterize the coupling relationship between the elastic and electrical polarization
effects of piezoelectric bulk. Dielectric constant (εr ) and dielectric loss (tan δ) are the other
factors to evaluate the convenience of polarization. The impedance spectrum is used to
obtain electromechanical coupling coefficients (Kt and Kp ) and further characterize the
mechanical–electrical conversion efficiency of the piezoelectric composites. The mechanical
quality factor (Qm ), describing the ability to overcome the energy consumed by internal
friction in the piezoelectric resonance state, is another critical parameter. Recently, lead-free
piezoelectric materials have been employed as function phases in CPCs, such as BT, BZT,
and BCTZO. Chaipanich et al. [68,71] employed the polarization-electric field loops (P-E
loops) to characterize the ferroelectric hysteresis properties of BT/BZT cement composites.
Considering the coupling complexity between the cement matrix and ceramics par-
ticles, a microstructural analysis of the composites was conducted to evaluate the op-
timization process. Jaitanong et al. [91] employed piezo-response force microscopy to
investigate the microstructure of the composite after hydration, thereby characterizing
the local piezoelectricity of the domains of PZT particles. Potong et al. [72] considered
the effect of the complex hydration condition and the various hydration products in the
cementitious material and applied linear voltage-differential transformer dilatometer to
test the thermal expansion, indicating that the thermal expansion the coefficient of the
composites with 30~70% BZT ceramic powder is similar to that of concrete. Wittinanon
et al. [39] evaluated the effect of PVDF on the composite’s mechanical properties using the
indentation technique. Moreover, acoustic impedance, porosity, and leakage current of the
composite with different PVDF content were also characterized [38].

3.3. Modelling Analysis

To understand the theoretical modeling, the size-dependent phenomenon of the CPCs
initially attracted attention. Wang et al. [92] consider the minor defect in the interface
(Figure 4) and proposed a modified micromechanics model to obtain the effective moduli
of particle-reinforced piezoelectric composites. The size effect, effective piezoelectric strain
σ− E f f
Ef f k33
factor (d33 ), and relative dielectric constant ( k0 ) are further discussed. Calculated
σ− E f f
Ef f k
results revealed a similar increasing trend of both d33 and 33k with the increase of
0
piezoelectric particle size. Meanwhile, the calculating and experimental results were in
good agreement, indicating that the micro-scale size effect exists. Attempting to investigate
the effect of pores and piezoelectric particles, Sladek et al. [93] investigated the effective
thermo-electro-mechanical material properties of CPCs based on the micromechanics’
representative volume element (Figure 5). The results illustrated the effective elastic,
and the piezoelectric coefficients are enhanced with the increase of piezoelectric particle
volume, while the effective heat and conduction coefficients are decreased. Additionally,
the increase of porosity will result in the effective elastic, piezoelectric, and heat conduction
coefficients decreasing.
 effective thermo-electro-mechanical material properties of CPCs based on the microme-
chanics’ representative volume element (Figure 5). The results illustrated the effective
effective thermo-electro-mechanical material properties of CPCs based on the microme-
elastic, and the piezoelectric coefficients are enhanced with the increase of piezoelectric
chanics’ representative volume element (Figure 5). The results illustrated the effective
Sensors 2021, 21, 3230
particle volume, while the effective heat and conduction coefficients are decreased. 10 Addi-
of 29
elastic, and the piezoelectric coefficients are enhanced with the increase of piezoelectric
tionally, the increase of porosity will result in the effective elastic, piezoelectric, and heat
particle volume, while the effective heat and conduction coefficients are decreased. Addi-
conduction coefficients decreasing.
tionally, the increase of porosity will result in the effective elastic, piezoelectric, and heat
conduction coefficients decreasing.

Figure
Figure 4.
4. Schematic
Schematicillustration
illustrationfor
forcomposite
compositematerials
materialswith
withimperfect
imperfectinterface [92].
interface. Reprinted with
permission from ref. [92]. Copyright 2016 IEEE.
Figure 4. Schematic illustration for composite materials with imperfect interface [92].

Figure 5. Finite element mesh of the porous PZT composite with the largest volume fraction [93].

Figure 5.
5. Finite
Finiteelement mesh of the porous PZT composite with the largest volume fraction [93].
Figure
3.4. Future Studyelement mesh of the porous PZT composite with the largest volume fraction.
Reprinted with permission from ref. [93]. Copyright 2006 Elsevier.
Based on
3.4. Future Studythe fundamentals and two-phase system, the complexity of the mechanical–
electrical
3.4. Futureconversion
Study process in the composite has been illustrated. Meanwhile, the local
Based on the fundamentals and two-phase system, the complexity of the mechanical–
strainBased
and field coefficients
on the fundamentals related totwo-phase
how the non-piezoelectric continuous
of the phase’s me-
electrical conversion process in andthe composite has system,
beenthe complexity
illustrated. Meanwhile,mechanical–
the local
chanical
electrical properties can dramatically affect the direct piezoelectric effect need further
strain andconversion processrelated
field coefficients in the composite
to how thehas been illustrated.
non-piezoelectric Meanwhile,
continuous the local
phase’s me-
study.
strain Experimental
and field studies related
coefficients on the microstructure
to how the of the composite
non-piezoelectric [52,62] have
continuous revealed
phase’s me-
chanical properties can dramatically affect the direct piezoelectric effect need further
the existence
chanical of defects
properties can in the ITZ between
dramatically thedirect
affect the ceramic particles and
piezoelectric effectmatrix due to insuf-
needhave
further study.
study. Experimental studies on the microstructure of the composite [52,62] revealed
ficient hydration,
Experimental resulting
studies on inmicrostructure
the poor local mechanical
of the properties[52,62]
composite and lower
have piezoelectric
revealed the
the existence of defects in the ITZ between the ceramic particles and matrix due to insuf-
properties.
existence ofWith
defectstheinemployment
the ITZ of finite
between the elementparticles
ceramic methods, andthe research
matrix due approach
to for
insufficient
ficient hydration, resulting in poor local mechanical properties and lower piezoelectric
piezoelectric
hydration, composite materials can be expanded. However, the complex microstructure
properties.resulting
With theinemployment
poor local mechanical properties
of finite element and lower
methods, thepiezoelectric properties.
research approach for
With the employment of finite element methods, the research approach
piezoelectric composite materials can be expanded. However, the complex microstructure for piezoelectric
composite materials can be expanded. However, the complex microstructure of composites
attributed to the material distinction and insufficient understanding of the mechanical
properties and microstructure after polarization may limit its simulation development.
The intense environment (higher voltage and temperature) during the polarization will
cause microstructural changes in cement products [94,95], and some damages due to the
chemical decomposition will lead to a decrease in mechanical properties. The mechanical
Sensors 2021, 21, 3230 11 of 29

and piezoelectric properties of the composite should be equally focused. The mechanical
properties of ITZ can dramatically affect the mechanical–electric response due to the stress
buffer between the piezoelectric ceramic particles and cement matrix. Further study on the
mechanical parameters (e.g., elastic modulus and Poisson’s ratio) of the composite after
polarization can promote the simulation development and understanding of its mechanism.

4. Materials for Cement-Based Piezoelectric Composites

In view of promoting the design and fabrication development of CPCs, it is essential
to understand the properties of the three different components: (i) function phase ma-
terials (piezoelectric materials), (ii) matrix phase materials (cementitious materials), and
(iii) enhanced phase materials (admixtures). The existence of the distinction in those raw
materials and the chemical reactions make the microstructure and chemical properties more
complex. For example, Dong et al. [96] reported the chemical reactions at the ITZ between
the piezoelectric particles and cement matrix, believing that there exists a coupling effect.
Wang et al. [52] found that the silicon-based materials can help obtain denser microstruc-
ture, thereby obtaining higher performance of the composite, and Cheng et al. [62] believe
that a higher hydration degree can obtain better piezoelectric performance. In this section,
reviewing the basic materials is conducted. By summarizing the considerations of related
materials, alternative materials for fabricating potential CPCs with better performance are
constructively provided, and the future study on materials for CPCs is also discussed.

4.1. Piezoelectric Ceramic for CPCs

Piezoelectric materials can be divided into three categories [34]: piezoelectric polymers,
piezoelectric composites, and piezoelectric ceramics. Piezoelectric ceramics have been
well-studied based on the solid solutions of lead-bearing materials (e.g., PbZrO3 (PZ),
PbTiO3 (PT)), and lead-free materials (e.g., BaTiO3 (BT)). Piezoelectric ceramic powder
for fabricating the CPCs are all ferroelectric materials, such as lead zirconate titanate
(PbTin Zr1-n O3 ; PZT) [48], barium titanate (BaTiO3 ; BT) [67], lead magnesium niobate
(xPb(Mgn Nb1-n )O3 -yPbTiO3 -zPbZrO3 ; PMN) [62], lead lithium niobate (xPb(Lin Nb1-n )O3 -
yPbTiO3 -zPbZrO3 ; PLN) and barium zirconate titanate (Ba(Zrn Ti1−n )O3 ; BZT). All of
them have perovskite-type structures, with the chemical formula ABO3 . The most used
piezoelectric material in SHM is PZT, which can be divided into soft and hard types. Due
to higher domain mobility leading to high sensitivity, soft PZT is regarded as an excellent
piezoelectric material for the sensing element. The special properties of the soft PZT include
the higher d33 and coupling factors. Generally, lead-bearing piezoelectric materials are
produced under high temperatures (about 800~1300 ◦ C) [63], which easily causes lead
volatilization and further results in the environmental problem. Due to eco-friendliness
issues, lead-free piezoelectric materials have received increasing attention to fabricating
the piezoelectric composites, such as BT, BZT, BCTZO, BNBK, and BNBT.
As the function phase, piezoelectric materials are the particle covered by the matrix,
directly endowing the composite with piezoelectric performance. Since cement-based
piezoelectric composite materials were proposed, the effect of the materials, content, and
size of piezoelectric particles on its final properties have been investigated, as summarized
in Table 3. It is clear to realize that the piezoelectric properties of Portland cement-based
composites usually increase with the increase of lead-bearing materials content at the
micro- and nano-level. The effect of size (ranging from 0.0236 to 620µm) on piezoelectric
performance has also been investigated. Huang et al. [82] evaluated the size effect on
piezoelectric properties and considered that the large particle (>100 µm) can insufficiently
affect the d33 and g33 . Li et al. [97] believed that the nano-powders with good crystallinity
and distribution in the cement matrix can prepare the composite with higher performance.
Hunpratub et al. [74] investigated the influence of BCTZO size and content and indicated
that the particles with a smaller size can obtain higher performance due to the better
connection. Kantakam et al. [78] characterized the dielectric properties of the geopolymer-
based composites, revealing that the increase of the ceramic particle content will lead to the
Sensors 2021, 21, 3230 12 of 29

decrease of ε r , but ε r is always greater than 1000, which may attribute to the influence of a
particular matrix. Apparently, the content and size of ceramic particles can dramatically
affect the density [70,98], which provides an approach to adjust the acoustic impedance.
The particle shape has also been considered. Jaitanong et al. [91] investigated the interface
and illustrated that the ceramic particles with angular shapes contribute to better bonding
properties. The influence of the size, content, and shape on the final piezoelectric properties
has been demonstrated. However, there are many other factors related to the material
contributing to the final performance, such as bonding with cement matrix, which is
difficult to summarize into a single problem, and the larger particles may lead to the loose
structure [98,99]. With the increase of the ceramic content, a lower cement content may
result in poor bonding behavior between the function phase and matrix. Therefore, the
appropriate piezoelectric particle should be considered further based on the total material
system. In summary, the larger particles and higher content are beneficial to improve
piezoelectric performance, while the oversize particles will lead to the lower performance
improvement efficiency, and the excessive content will cause bonding defects.
Sensors 2021, 21, 3230 13 of 29

Table 3. Properties of cement-based piezoelectric composites with different piezoelectric ceramic particles content and size.

Piezoelectric Particle
Cement Properties Findings References
Content Size
Type
(%) (µm)
35~70 vol. 6.45 (mean) PZT Portland cement d33 /ε r /Kt ↑• g33 ↑•  40~50 vol.% of ceramics is the optimal content for matching Li et al., 2002 [34]
35~65 vol. 153.6 (mean) acoustic impedance of concrete.
80 wt. 0~300 (mean) d33 ↑•  High polarization field (<4kV/mm)/temperature (<130 ◦ C) Huang et al., 2004 & 2005
60~85 wt. PZT/PMN Sulphoaluminate cement K p /Kt /g33 ↑•
166.5 (mean) and increased polarization time (<45min) lead to the [46,62]
18~50 vol. 153.6 (mean) PZT Portland cement d33 ↑• enhanced performance. Li et al., 2005 [61]
1.45/2.34/9.03/  d33 increases with the curing time.
27.17/35.97/43.46/ d33 /g33 /Kt /Kp ↑•  Larger PLN particles lead to the change of connectivity
80 wt. PLN Cement Huang et al., 2006 [82]
58.43/68.51/107.08/294.07 Qm ↓ patterns; large particle (>100µm) can insufficiently affect
(mean) the d33 and g33 .
620 (median)  Less contact area between the cement matrix and the PZT
40~60 vol. PZT d33 /ε r ↑•
50 vol. 3.8/148.8/620 Portland cement tan δ↓• Chaipanich et al., 2007 [47,80]
(median) particles enhance the piezoelectric properties.
50~70 vol. 300~600 PSZT Portland cement ε r /d33 /Kt ↑•  PZT modified by Sr and Sb can obtain better piezoelectric Chaipanich et al., 2009 [100]
tan δ↓• performance.
 PZT nano-powders with good crystallinity and
35~80 vol. 0.0236 (mean) PZT Portland cement d33 /Kt /ε r ↑• high-quality network distribution in cement can obtain Li et al., 2009 [97]
good piezoelectric performance.
30~50 vol. 425 (median) PZT Geopolymer tan δ/ ε r ↓•  The ε r can reach 1017.6~1834.2, different from that of Kantakam et al., 2013 [78]
tan δ↓ Portland and sulphoaluminate cement.
40~70 vol. 425 (median) BZT ε r /Kt /d33 /Zc/ ρc  Acoustic impedance and density increase with size and
Portland cement Potong et al., 2013 [70,71]
50 vol. 75/212/425 (median) content increasing.
↑•
30~70 vol. 425 (median) Kt/ Zc ↑•  Acoustic impedance increases with increasing particle size
BT Portland cement and content, while porosity decrease with larger particle. Rianyoi et al., 2013 [67]
50 vol. 75/212/425 (median) P*↓
 A higher specific surface and lower interface space can lead
ε r ↑• to better connection in ceramic particles.
30~70 vol. 8.9/569.8 (mean) BCTZO Portland cement d33 ↓, ↑•  Low polarizations for smaller particles resulting in a lower Hunpratub et al., 2014 [74]
tan δ ↓•
dielectric constant.
BT P*↓• Zc ↑•  Acoustic impedance increases while porosity decrease with
40~60 vol. 425 (median) Portland cement ε r ↑• tan δ↓• Wittinanon et al., 2020 [38]
increasing particle content.
↑•: increase with the particle content increasing; ↑: increase with the particle size increasing; ↑•: increase with both the particle size and content increasing; ↓•: decrease with the particle content increasing;
↓: decrease with the particle size increasing; ↓•: decrease with both the particle size and content increasing; P*: porosity; Zc : acoustic impedance; ρc : density.
Sensors 2021, 21, 3230 14 of 29

4.2. Matrix of CPCs

Polymers were usually employed as the matrix of piezoelectric composites [101,102]
for the sensing element. Some natural defects exist in polymer/piezoelectric composite,
such as the compatibility issue between the polymer and ceramics due to the significant
difference in their composition and aging. The compatibility between the host material and
the inbuilt sensing element has been another issue, attracting increasing attention. Cement,
as an inorganic material, with excellent durability, can be mixed with piezoelectric particles
directly, thereby obtaining inorganic composites. Cement-based piezoelectric composite
can match the acoustic impedance and mechanical properties of concrete, more applicable
to concrete-based infrastructure. However, the complex microstructure of the cement
caused by the hydration products, porosity, long-term physical changes, and chemical
reaction leads to an adverse impact on CPCs in the fabrication process, polarization process,
and final performance.
Additionally, the occurrence of ITZ in the composite with weakened bonding behavior
due to the difference in the growth rate of hydration products (e.g., CSH gel and calcium
hydroxide crystal) is also a challenge. Different cement types have different chemical
processes and durations, which requires selecting the curing condition and duration based
on cement properties in the fabrication process. It is a delicate issue of CPCs between the
cement matrix and piezoelectric materials that the higher temperature can help obtain
the better piezoelectric properties but destroy the cement matrix due to chemically bound
water loss. In the polarization process, the decomposition of chemically bound water
caused by the high temperature and the product structure changes due to the extremely
high voltage can increase the volume content of porosity and lead to the matrix strength
loss. One issue for CPCs is that the matrix fabricated by various cement leads to the
distinction in its final piezoelectric performance [47]. Each type of cement consists of a
different component, resulting in the hydration products presenting specific forms, thereby
affecting the final performance. Another issue is that specific types of cement, which with
excellent properties including but not limited to high conductivity, high strength, and low
porosity, such as geopolymer, can be an alternative matrix material. Due to the component
difference in different cement types, further studies about the influence of cement type on
the CPCs should be carried out. Tables 1 and 2 show that the geopolymer-based composites
show a higher dielectric constant and the inverse trend of piezoelectric performance by
mixing higher-volume fractions of ceramic particles, which is an excellent inspiration to
develop CPCs with various cementitious materials as a matrix.
Up to now, Portland, sulphoaluminate, and geopolymer cement have been employed
to fabricate the composite. Additionally, to mitigate the mismatching, Zhao et al. [57]
prepared the cement-sand-based piezoelectric composite, believing that it can improve
mechanical strength, despite leading to a low-efficiency polarization process. This study
also shows the difference in performance brought from the matrix. Although some studies
about the influence of the matrix properties [48,78] have been carried out, it is still difficult
to control the effect of the matrix on the performance of composite materials due to the
complexity of the hydration characteristics of cement materials and the sensitivity of
bound water to high temperatures. Concrete materials can self-heal [103] due to secondary
hydration, carbonation, etc. This ability may contribute to the performance variation
with time. Aging, related to the degradation with age after polarization, is caused by the
releasing behavior of internal stress and redivision of ferroelectric domains, which is one of
the major factors determining the stability of the piezoelectric performance. Dong et al. [37]
found that the d33 of polymer-based composites after aging show a decreasing trend, while
the d33 of CPCs show an increasing trend. Wang et al. [52] believed that the d33 could
increase after polarization until the hydration process is completed. Considering the
adverse impact of the free water on the polarization process, Pan et al. [83] pointed out
that the d33 of CPCs with the high-temperature treatment can reach stable values earlier.
However, the excessively high-temperature treatment can easily change the chemically
bound water to free water, resulting in the matrix defects. It illustrates that the influence of
Sensors 2021, 21, 3230 15 of 29

water on the polarization may be more significant than that of defects. Additionally, some
studies demonstrate that the direct piezoelectric effect can be characterized in hardening
cement paste [104] and geopolymeric mortar [105] due to the presence of water, but there
is no evidence to prove the contribution of the matrix to the piezoelectric effect. Although
the composite’s aging shows a positive impact on the piezoelectric performance, it may
lead to the uncontrolled final performance.
Currently, several issues related to the matrix have been investigated, as summarized
in Table 4, which can be classified into (a) ITZ, (b) mechanical properties, (c) leakage
current, (d) fabrication period, and (e) performance variance. The matrix properties mainly
determine the ITZ, adequate curing promotes the cement to obtain a higher hydration
degree and the admixture contributes to a denser matrix, thereby optimizing the ITZ and
reducing defects. Compared with the ceramics and cement, the elastic modulus of cement
is much lower. Adding admixture with higher elastic modulus is an excellent approach
to modify the mechanical properties. A complex issue is that the polarization process
can endow the ceramic with piezoelectric properties while causing damage to the matrix.
Meanwhile, the ions and pores in the matrix may result in the occurrence of leakage current.
Although the higher temperature and stronger electric field can destroy the matrix, it can
help obtain better piezoelectric performance. Cheng et al. [95] considered the appropriate
polarization temperature based on the decomposition temperature of hydrated cement and
characterized the performance in various time and electric fields; Pan et al. [60] considered
the moisture effect on CPCs and performance per-heat treatment, thereby obtaining lower
dielectric losses; Wittinanon et al. [38] modified the microstructure of matrix by mixing
PVDF, and the leakage current reduced dramatically. Although the variety of piezoelectric
performance caused by long-term hydration of cement has been realized and promotes
the utilization of quick-setting cement, fewer studies illustrate its advantage. Due to
aging and the interference of piezoelectric ceramics on the cement hydration [77], the final
performance is difficult to predict.

4.3. Admixture for CPCs

Generally, obtaining a denser matrix and improving the conductivity and mechanical
properties are the basic ideas for selecting admixture. The effect of admixture on the
piezoelectric performance of CPCs is summarized in Table 5. The lower piezoelectric per-
formance is a common issue in piezoelectric composites, and the improvement of d33 with
admixture is the most noteworthy. The electromechanical coupling coefficient (Kt and Kp )
and dielectric constant (εr ) were also characterized. Many admixtures have been studied,
showing the complex relationship between the piezoelectric performance and admixtures
content. The excess electric conductivity will reduce the piezoelectric activities [55,56].
Meanwhile, the piezoelectric performance optimization by pozzolanic materials after a
long period was also observed. Currently, the admixture mainly includes carbon materials,
pozzolanic materials, and polymer. According to Table 5, these materials could improve
the final performance efficiently, while excessive additives would cause performance degra-
dation. The distinction of admixtures in physical and chemical properties, such as size,
shape, and component, can lead to a significantly different performance. With the in-depth
understanding of this composite, the research on the acoustic impedance and mechanical
properties of admixture has gradually been paid more attention. There is a negative effect
on piezoelectric performance caused by the distinction of elastic modulus between cement
and piezoelectric ceramic particles. Concerning the efficiency of stress transfer between
the matrix and ceramic particles, basalt fiber [43] is employed to improve the matrix’s
elastic modulus and mitigate the stress buffer, thereby increasing the mechanical–electrical
response. Admixture usually can positively impact the matrix compactness, thereby af-
fecting the overall mechanical properties and acoustic impedance. Wittinanon et al. [38,39]
revealed that PVDF could simultaneously control the piezoelectric properties, mechanical
properties, and microstructure.
Sensors 2021, 21, 3230 16 of 29

Table 4. Effect of cementitious matrix on the performance of CPCs.

Issues Factors Approach Findings References

• Higher hydration
ITZ between degree contributes to  Better curing  Adequate during period lead to
cement matrix better ITZ method and better ITZ and higher d33 [62]. Cheng et al., 2005 [62]
and ceramic • Cement component adequate curing  Better microstructure is Wang et al., 2012 [52]
particles time
and hydration  Adding admixture obtained [52].
products [52]
• Lower elastic  Admixture with high modulus
modulus and the good bonding interface
• Lower mechanical with cement enhances local
Mechanical  Adding admixture stress [43], thereby improving Zhang et al., 2019 [43]
strength
properties  Matrix with high piezoelectric performance. Zhao et al., 2016 [57]
• Mismatching of
elastic modulus  Adding sand as a part of matrix
mechanical
properties between obtains higher mechanical
cement and ceramics strength [57].
 Polarization temperature for
sulphoaluminate cement should
• Chemically bonding  Select the be lower than 130 ◦ C, thereby
water decomposes at appropriate reducing the loss of crystal water,
Chen et al.,
high temperature polarization and meanwhile 45min for 2004 [46] & 2006 [95]
Leakage cur- [46] temperature, field, polarization is efficient; it is easy Pan et al., 2016 [60]
rent/conductivity • Free water and time to breakdown if polarization Wittinanon et al.,
• Pores  Per-heating field is over 4 kV/mm [95]. 2020 [38]
• Weakly conducting treatment  Less free water leads to better
ions  Adding admixture piezoelectric performance [60].
 PVDF fills the pore and reduces
the leakage current [38].
Fabrication period • Slow hydration  Quick-setting  Prepare CPCs with Huang et al., 2007 [59]
process cement as matrix sulphoaluminate cement [59].
 The decrease of porosity leads to
better stress transformation at
first 90 days after polarization
and enhance the d33 [52].
 Continue hydration may lead to
• Aging the increase of d33 [63]. Wang et al., 2012 [52]
Performance • Existence of  Performance testing  Charge redistribution in CPCs Chaipanich et al.,
variance ceramics hinder until stable partly attribute to the age and 2014 [63]
hydration [77] Pan et al., 2020 [64]
w/c [64]. Santos et al., 2020 [77]
 Cement curing process
contributes to unstable dipoles
and piezoelectric phase
constriction, resulting in aging
fluctuations [77].
Sensors 2021, 21, 3230 17 of 29

Table 5. Influence of admixture on the performance of CPCs.

Admixture Content (%) Matrix Piezoelectric Ceramic Properties Consideration Major Findings References

• Dense matrix  Silica fumes make the matrix dense and improve
Silica fume 5~10 wt. Portland cement PZT d33 / ε r ↑ piezoelectric performance. Chaipanich et al., 2007 [51]

Carbon addition 1~2 vol. Portland cement PZT ε r /tan δ ↑ • Continuous electric flux  Carbon addition improves the dielectric behaviors. Jaitanong et al., 2008 [54]
d33 /g33 ↑ • Conductivity  Excessively high conductivity leads to poor
Carbon black 0~1 vol. Sulphoaluminate cement P(LN)ZT Kt/Qm = piezoelectric performance. Huang et al., 2009 [55]
d33 /Kt /Kp ↑ • Conductive phase  Excess electric conductivity leads to lower
Carbon black 0~1.7 vol. White cement PZT piezoelectric activity. Gong et al., 2009 [56]
ε r /tan δ%&
d33 /g33 %&
• Conductive filler improves the
Carbon nanotubes 0.1~1.3 vol. Portland cement PZT  CNTs increase the polarization efficiency. Gong et al., 2011 [81]
ε r /tan δ ↑ polarization efficiency
 The d33 of silica-based composite (20 wt.%) cured at
d33 ↑→↑
• Enhanced phase
Silica-based material 10~20 wt. Portland cement PZT room temperature and dry atmosphere can reach Wang et al., 2012 [52]
εr ↑ • Optimize the ITZ
70pC/N after 38 days.
 The performance test results at a later period after
• The performance changes with polarization are more suitable as a representative
10~50 wt. PZT d33 / ε r /g33 →↓ time value.
Slag Fly ash Portland cement Pan et al., 2014 [49]
Kt →= • Improve the strength of matrix  Curing time shows little effect on the final
performance.
d33 %&,→↑ • The performance changes with
Fly Ash 10~50 vol. Portland cement PZT g33 %&,→↓ time - Pan et al., 2014 [106]
ε r →↑
• Being as a connecting third  Adding PVDF to the composite significantly reduces
d33/ g33 / ε r /tan δ phase with desirable properties
PVDF 1~20 vol. Portland cement PZT polarization time. Jaitanong et al., 2014 [107]
%& • To promote polarization
ε r →↑,↑
tan δ ↑ • Enhance ferroelectric behavior  The composite mixed with kaolin reduces the porosity.
Kaolin 0~10 vol. Portland cement PZT Pan et al., 2015 [53]
d33 →↑,↓
Kt→=, ↑g33 =
Carbon nanotubes Portland cement and d33 / ε r %&
• Increase electrical conductivity  Composite mixed with CNTs can be used to catch the
0~0.9 vol. PZT for easier polarization stress changes. Zhao et al., 2016 [57]
(CNTs) sand tan δ ↑
• Increase electrical conductivity  CNTs optimize the microstructure and improve the
BNBK d33 /g33 %&
Carbon nanotubes 0~2 vol. Portland cement for easier polarization piezoelectric properties. Potong et al., 2017 [76]
ε r /tan δ ↑
• Evaluate the effect of GNPs on
 There is no particular concentration of GNPs,
Graphene nanoplatelets Silica fume blended morphological and electrical
0~5 wt. PNZT ε r /tan δ ↑ enhancing the dielectric behavior. Jaitanong et al., 2018 [58]
(GNPs) Portland cement properties

ε r /tan δ↓ • Efficient polarization  Adding PVDF obtains a denser matrix.

PVDF 1~10 vol. Portland cement BNBT Rianyoi et al., 2018 [75]
d33 %&
 The density decreases and inadequate reaction of
ε r ↓tan δ ↑ • Improve physical properties of cement caused by excessive fly ash content led to the
Fly ash 10~50 vol. Portland cement BZT matrix Chomyen et al., 2018 [50]
d33 /D↓ decrease of piezoelectric properties.
 Local stress is significantly enhanced by BF with high
V*/g33 %& • Increase elastic modulus of
Basalt fibers (BF) 0~0.24 vol. Portland cement PZT matrix modulus and good interface bonding with cement Zhang et al., 2019 [43]
tan δ/ε r %& d33 ↓ matrix.
• Evaluate the effect of PVDF on
ε r ↓ d33 %& microstructure, physical,  PVDF can optimize the physical, dielectric and
PVDF 0~7 vol. Portland cement BZT P*/Hv /Hk /E↓ mechanical and piezoelectric piezoelectric properties by increasing densities. Wittinanon et al., 2020 [39]
Kc ↑ properties
• Evaluate the effects of PVDF on  Adding PVDF can optimize the microstructure,
ε r /tan δ↓ the density, porosity, control acoustic impedance, and reduce porosity and
PVDF 0~7 vol. Portland cement BT g33 /d33 %& microstructure, acoustic Wittinanon et al., 2020 [38]
P*/Zc/ A↓ impedance, dielectric and leakage current.
piezoelectric properties

↑: increase with the admixture content increasing; ↓: decrease with the admixture content increasing; =: slight fluctuation with the admixture content increasing; %&: increased first and then decreased with the
excess admixture content increasing; →↑: increase with time (at the same content of admixture); →↓: decrease with time (at the same content of admixture); →=: slight fluctuation with time (at the same content
of admixture). P*: porosity; V*: output voltage; Hv : Vickers hardness; Hk : Knoop hardness; E: elastic modulus; Kc : fracture toughness; Zc : acoustic impedance; A: leakage current; D: density.
Sensors 2021, 21, 3230 18 of 29

4.4. Further Study on Materials

The material selection can fundamentally determine the fabrication process and dra-
matically affect the final performance. Selecting materials should consider factors including
the material availability and uniformity, piezoelectric performance, and convenient fabrica-
tion. In terms of piezoelectric materials, PZT has been widely used as a common material
for CPCs. Lead-free piezoelectric materials are a promising candidate for the function phase
of composite. The chemical reaction between piezoelectric ceramic and cement [96] can
enhance the interface via chemical bonding. A case study on polymer/piezoelectric ceramic
by Zheng et al. [108] has demonstrated the efficiency in improving piezoelectric perfor-
mance by enhancing interface bonding with chemical reaction. Therefore, an optimization
strategy is to modify the surface of piezoelectric ceramic particles, enhancing bonding. As
the matrix phase, cement can also dramatically affect the piezoelectric properties. Scholars
have employed some eco-friendly cementitious materials (e.g., geopolymers, magnesium
phosphate cement), showing good durability and mechanical properties and controllable
setting-time, which can be the potential matrix. Admixture is usually regarded as the
material phase with an adjustment effect to optimize the mechanical and piezoelectric
properties. The chemical reaction between the piezoelectric ceramic and cement matrix
may occur in their ITZ, and the stress buffer [43] in ITZ leads to a low local piezoelectric
strain factor. Further studies should investigate the mechanical properties and chemical
bond of the composite, especially in the ITZ.

5. Fabrication Process of CPCs

5.1. General Fabrication Process
The fabrication process of CPCs is related to shaping the composite, modifying the
microstructure, and reactivating the electrical response. The process mainly includes: (i)
mixing, (ii) forming, (iii) curing, (iv) polishing, (v) coating, (vi) drying (heat treatment), and
(vii) electrode forming and polarization. The (i)~(vi) steps can be called the preparation
process, while the (vii) step is regarded as the polarization process. The preparation process
relates to the shape of materials; the polarization process is in terms of functionalization.
In polarization, the extreme temperature and electrical treatment process can cause certain
matrix defects. In turn, the original defects of CPCs can adversely impact the electrical
response efficiency, even resulting in a composite scrap [95]. Preparation parameters have
a profound impact on CPCs, and although those parameters can be considered based on
the properties of the materials, there are still some issues that can adversely impact the
final performance.

5.2. Preparation Process

During the preparation process, the forming, curing, and drying (heat treatment),
show a significant influence on the mechanical properties and later functionalization.
Considering the defect caused by the conventional grouting molding method and the
natural pores of cement materials, the compression molding method was employed to
modify the microstructure, and later the influence of the forming pressure on piezoelectric
properties was studied [59]. Due to the improvement of piezoelectric properties, the
compression molding method became a major molding method for fabricating CPCs,
deeming that the denser matrix can be obtained. However, excessive pressure will lead
to internal micro-cracks, thereby lowering the density. Subsequently, the curing process
for cement hydration is essential, which could improve the integrity of CPCs due to the
chemical bonding and chemical reaction between the cement matrix and ceramic [96]. The
free water will reduce during the drying process [60], improving the polarization efficiency.

5.3. Functionalization Process

Piezoelectric ceramics for CPCs are the artificial polycrystalline materials, with electric
domains arranged in arbitrary orientation inside the micron-level grains, displaying no
piezoelectricity macroscopically before polarization. To obtain the macroscopic piezoelec-
Sensors 2021, 21, 3230 19 of 29

tricity, the higher temperature, mechanical stress, or electric field can be employed to
change the domain structure (also called dipole line-up), reversing the 180◦ domain and
rotating the 90◦ domain. Generally, an electric field combined with increased temperature
(below the Curie temperature) is regarded as a suitable approach to help piezoelectric
ceramics generate the macroscopic polar axis and piezoelectricity easily, even though it will
lead to the internal crack. For CPCs, the polarization is the same as pure piezoelectric ce-
ramics, but the negative impacts are more complex due to the cement matrix and additives.
Electric field, temperature, and polarization time are the major factors for the piezoelectric
performance, but firstly, the electric field is the essential condition to be considered.
The local electric field (E1 ) on the piezoelectric particles of CPCs and the average
electric field (E2 ) on the matrix can be expressed as [81,102].
This is example 1 of an equation:

3ε 2
E1 = E0 , (29)
ε 1 + 2ε 2

E2 = E0 , (30)
where ε 1 and ε 2 are the dielectric permittivity of piezoelectric particles and cement matrix,
respectively; E0 is the external electric field.
Additionally, based on the molecular level mechanism, Li et al. [109] illustrated the
relationship between the dipole domains of piezoelectric ceramic particles and macroscopi-
cal parameters of CPCs. This mechanism reveals the polarization efficiency, which can also
help understand the relationship between the polarization and macroscopic piezoelectricity.
The description of the mechanism is [109]:

P = κ 0 − 1 ε 0 E = NαE0 ,


(31)

where P is the polarization, equal to the dipole moment of each unit volume of the piezo-
electric ceramics; κ 0 is the relative dielectric constant of piezoelectric ceramics; ε 0 is the
permittivity of vacuum; N is the number of the contribution elementary particles per
unit volume; α is the polarizability; E0 is the local electric field; E is the applied electric
field. From Equation (29), E1 depends on the dielectric permittivity of the piezoelectric
particle and cement matrix. Equation (30) reveals the strong electric field applied to the
matrix. The much higher ε 1 and lower ε 2 can lead to the smaller E1 during polarization.
Additionally, Equation (31) describes the direct relationship between the applied electric
field and macroscopic piezoelectricity, while P describes the macroscopic piezoelectricity
from the molecular level, representing the charge density on the surface. From Table 2, it
is clear that the ε 1 that have been applied in CPCs range from about 1000 to 3600, while
ε 2 is about 40 to 530, which leads to the lower d33 , and the appropriately high electric
field density can help achieved a higher piezoelectric performance (Figure 6a). The d33 is
directly related to the electric field, and the higher electric field intensity can help obtain a
higher d33 . However, the migration of weakly conductive ions (OH− , Ca2+ , etc.) [95] in the
cement matrix under the applied electric field will cause the decrease of breakdown voltage,
which possibly leads to polarization failure. The excessive polarization time can also lead
to inefficient polarization even though the appropriately high electric field was carried
out. Dong et al. [61] characterized the negative effect of long polarization time on the
piezoelectric performance (Figure 6b) and considered that a part of saturated piezoelectric
particles has been broken down. Figure 6 also indicates the improvement of d33 with age,
which seems to be contrary to the characteristics of piezoelectric ceramics. Chaipanich
et al. [63] believed that the remnant polarization of the piezoelectric particles will reduce
with time because the 90◦ ferroelectrics domains gradually become disordered, but the
hydration of cement after polarization can densify the matrix, thereby improving the d33 .
 Sensors 2021, 21, x FOR PEER REVIEW 21 of 31

Sensors 2021, 21, 3230

al. [63] believed that the remnant polarization of the piezoelectric particles will reduce
20 of 29
with time because the 90o ferroelectrics domains gradually become disordered, but the
hydration of cement after polarization can densify the matrix, thereby improving the d33.

(a) (b)
Figure
Figure 6. (a)
6. (a) TheThe effect
effect ofof polarizingvoltage
polarizing voltageon
ondd3333 for
for 0-3
0-3 type
type cement
cementbased
basedPZT
PZTcomposites
composites. [61], (b) The effect
Reprinted with of polar-
permission
izing
from ref.duration on d33 for
[61]. Copyright 0-3 Elsevier.
2020 type cement-based PZTofcomposites
(b) The effect polarizing [61].
duration on d33 for 0-3 type cement-based PZT composites.
Reprinted with permission from ref. [61]. Copyright 2020 Elsevier.
The microstructure of CPCs will change under the applied electric field and higher
temperature during the polarization
The microstructure of CPCs willprocess.
changeCurrently,
under thethe polarization
applied electrictemperature of
field and higher
CPCs with lead-based piezoelectric ceramic is about 80~160 °C, which could
temperature during the polarization process. Currently, the polarization temperature lead to the
ofinstability
CPCs with of crystal waterpiezoelectric
lead-based in hydration ceramic
products is(CSH gel,80~160
about Al2O3·3H 2O, etc.). Further-
◦ C, which could lead
more, the occurrence of chemical reactions and water loss would result in additional in-
to the instability of crystal water in hydration products (CSH gel, Al 2 O3 ·3H2 O, etc.).
ternal defects. Under the applied electric field, weakly conductive ions (OH−, Ca2+, etc.)
Furthermore, the occurrence of chemical reactions and water loss would result in additional
[95] in the matrix will accumulate at defects, pores, and ITZ, thereby generating an oppos-
internal defects. Under the applied electric field, weakly conductive ions (OH− , Ca2+ ,
ing electric field and resulting in polarization suppression [59]. Chaipanich et al. [71] char-
etc.) [95] in the matrix will accumulate at defects, pores, and ITZ, thereby generating
acterized the ferroelectric hysteresis of cement-based BZT composites at room tempera-
an opposing electric field and resulting in polarization suppression [59]. Chaipanich
ture, and the polarization-electric field loops (P-E loops) show a lossy feature, which was
et al. [71] characterized the ferroelectric hysteresis of cement-based BZT composites at
also inferred to be the result of weakly conductive ion migration. The electric field can
room temperature, and the polarization-electric field loops (P-E loops) show a lossy feature,
also produce a polarization effect in the cement matrix and change its electric dipoles
which was also inferred to be the result of weakly conductive ion migration. The electric
alignments (see Figure 7) because calcium-silicate-hydrate (CSH) can obtain a better uni-
field
formcan also produce
nano-scale a polarization
morphology and then effect
reduceinthethe
ioncement matrix and
transportability, change
thereby its electric
enhancing
dipoles alignments (see Figure 7) because calcium-silicate-hydrate (CSH)
the output voltage. However, the contribution of electric treatment to the piezoelectric can obtain a
better uniform nano-scale morphology and then reduce the ion transportability,
properties of CPCs is limited, even leading to some mechanical issues. A strong electric thereby
enhancing the output voltage. However, the contribution of electric treatment
field and the ions in the pores could lead to the directional structure, inspiring further to the
piezoelectric properties of CPCs is limited, even
study on the matrix’s microstructure after polarization. leading to some mechanical issues. A
strong electric field and the ions in the pores could lead to the directional structure, inspiring
further study on the matrix’s microstructure after polarization.
The high temperature would mitigate the suppression effect, reducing the cement
matrix’s resistivity, thereby improving the polarization efficiency. It could also enhance the
electric domain rotation and more easily realize directional array under the applied electric
field, thereby obtaining better piezoelectricity. Meanwhile, a higher temperature could
reduce the electric domain’s obstruction in the turning process and make the polarization
process much easier in a relatively lower voltage. However, the defects caused by the
chemical reaction under a higher temperature would generate the loose matrix and increase
ion transportability, which further led to the decrease of the matrix resistance and resulted
in the CPCs breakdown in an applied electric field. Lead-free piezoelectric materials
have been employed in the composites, performing the polarization at the temperature of
60~80 ◦ C, which could reduce the matrix damage.
We summarized the performance and polarization parameters of CPCs with different
piezoelectric ceramic types in Table 6. Due to the almost identical piezoelectric particle size
and content, and cement type, the final performance and fabrication parameters are easy to
Sensors 2021, 21, 3230 21 of 29

be compared. The d33 of lead-bearing and lead-free materials (with about 425 µm mean
particle size) are similar, while the temperature and electric field for lead-free materials
is lower than that of lead-bearing materials. For lead-free materials, although the low
Curie temperature and thermal stability are the disadvantages affecting the composite
application in severe environments, the lower polarization temperature could reduce its
effect on the matrix. When the temperature is over 80 ◦ C, the bound water of Portland
Sensors 2021, 21, x FOR PEER REVIEW 22 of 31
cement will be lost. A lower temperature can mitigate the damage and water loss, thereby
improving the density of the composite.

Figure 7. Atomic Figure 7. Atomic (AFM)

force microscopy force microscopy (AFM) and
for non-polarized for non-polarized andReprinted
polarized cement. polarized with
cement [79].
permission from ref. [79].
Copyright 2019 Elsevier.
The high temperature would mitigate the suppression effect, reducing the cement
matrix’s resistivity,
Table 6. Performance thereby
and polarization improving
parameters the polarization
of CPCs with different efficiency. It could also enhance
ceramic type.
the electric domain rotation and more easily realize directional array under the applied
Piezoelectric Ceramics Fabrication
electric field, thereby obtaining better piezoelectricity. Meanwhile, a higher temperature
Cement Forming Curing
Particle Electric d33 (pC/N)
Ceramics
Size
Content TypecouldAdmixture
reduce the Pres-
electric domain’s
Time/ obstruction
Temperature in the turning
Field
Time process
εr
and make
tan δ the polar-
References
Type (vol. %) sure Temperature (◦ C) (min)
(µm) ization process much (MPa) easier in C)
(day)/( ◦ (kV/mm)
a relatively lower voltage. However, the defects caused by
the chemical reaction under a higher temperature would generate the loose matrix and
Chaipanich
PZT 620 50 OPC et al.,
increase Nion transportability,
80 3/60
which further 130 2
led to the 45
decrease 176
of the26matrix0.79 resistance
2007&2008and
[47,80]
resulted in the CPCs breakdown in an applied electric field. Lead-free piezoelectric mate-
Chaipanich
PZT 450 50 OPC N - 3/60 130 2 45 120 17 - et al., 2007
rials have been employed in the composites, performing the polarization at the tempera- [51]
Potong
BZT 425 50 OPC
ture of 60~80
N
°C, which
-
could
3/60
reduce the50
matrix damage.
1 45 350 14 0.87 et al., 2013
We summarized the performance and polarization parameters of CPCs with differ-
[70,71]
Hunpratub
BCTZO 569.8 50 OPCent piezoelectric
N ceramic
146 types
3/60 in Table R* 6. Due to the 1 almost 45 identical
80.7 18piezoelectric
0.1 etparticle
al., 2014
[74]
size and content, and cement type, the final performance and fabrication parameters Potongare
BNBK 425 50 OPC N - 3/60 80 1.5 45 188 41 ~0.7 et al., 2017
easy to be compared. The d33 of lead-bearing and lead-free materials (with about 425μm [76]
Chomyen
BZT 425 50 OPCmean particle
N size)- are similar,
3/60 while the 60 temperature
0.5 and
45 electric field for0.73lead-free
1220 16.28 ma-
et al., 2018
terials is lower than that of lead-bearing materials. For lead-free materials, although [50] the
Rianyoi
BNBT 425 50 OPClow Curie N temperature- and3/60
thermal stability 60 are 0.5
the disadvantages
45 ~300 ~26affecting ~0.6 theetcompo-
al., 2018
[75]
site application in severe environments, the lower polarization temperature could reduce
Wittinanon
BT 425 50 OPC N - 3/60 60 1 45 249 17 0.66 et al.,2020
its effect on the matrix. When the temperature is over 80 °C, the bound water of Portland [38]
cement
R*: polarization in will be lost.
room temperature; A lower
N: without temperature
admixture; -: cannot can mitigate
obtain accurate the damage
value and water loss, thereby
from literature.
improving the density of the composite.
Therefore, a suitable temperature and electric field can be considered as coupling coupling
conditions, essential for the piezoelectricity activation of CPCs. The fewer internal defects
(pores, ITZ,
ITZ, etc.)
etc.)could
couldalso
alsosignificantly
significantly contribute
contribute to to
thethe polarization
polarization efficiency.
efficiency. TheThe po-
polarization
larization process
process parameters
parameters should
should considerthe
consider theeffect
effectofofions
ionsandandpores
pores in in the matrix
because it can result in the local piezoelectric performance difference. Pre-heating may be
an appropriate approach to reduce the water in the matrix to address the interference is-
sue between the temperature and electric field. The material type is also another factor
contributing to the parameter selection, especially the ceramic type.
Sensors 2021, 21, 3230 22 of 29

because it can result in the local piezoelectric performance difference. Pre-heating may
be an appropriate approach to reduce the water in the matrix to address the interference
issue between the temperature and electric field. The material type is also another factor
contributing to the parameter selection, especially the ceramic type.

5.4. Future Study on Fabrication

According to different material characteristics, it is essential to select the reasonable
forming pressure and curing mode and optimize the fabrication process based on the dif-
ferent material types. Concerning the significant effect of stable piezoelectric performance
on the composite as a sensing element, the approach to accelerate the aging period is
essential. After polarization, the further hydration of the cement matrix is the major reason
for the increase of piezoelectric properties with age, which enlightens the post-processing
exploitation to stabilize the piezoelectric property quickly. High-temperature curing could
be a potential approach. There are some challenges in considering fabricating the com-
posite with eco-friendly materials and a faster preparation process. A good advantage
of lead-free barium zirconate titanate for the composite is low-temperature polarization.
Like geopolymer, some new types of cement with good dielectric properties can be the
promising matrix. Recently, 3D printing is one of the potential manufacturing approaches
and has been employed in sensor design and manufacturing [110]. The application of addi-
tive manufacturing technology in polymer-based piezoelectric composites’ [108] structure
design and preparation also proves the feasibility of the piezoelectric composites combined
with additive manufacturing technology, attributed to its good flexibility, and easy pro-
cessing and molding, showing a promising prospect in combining smart manufacturing
technology with sensor fabrication. Song et al. [111] employed 3D printing to prepare novel
aggregate-shape embedded piezoelectric sensors. Chen et al. [112] fabricated a focused
ultrasonic array with BaTiO3 ceramics via 3D printing, showing a good advantage in the
size and shape control of piezoelectric ceramics. Lejeune et al. [113] fabricated piezoelectric
ceramic with micro size by 3D printing. Considering the importance of the shape and
size of piezoelectric particles for CPCs, this technique can be an approach to support the
composite with controllable piezoelectric performance.

6. Application of CPCs
6.1. Application of CPCs
The application of the cement-based piezoelectric composite using various techniques
is listed in Table 7. Considering the excellent compatibility of CPCs with concrete struc-
ture, the composites were encapsulated as the sensing element, namely cement-based
piezoelectric ceramic composite sensor, which has been employed to monitor several is-
sues, including cracking, steel corrosion, deterioration, and the hydration process. Those
studies cover the issues encountered in the life cycle of concrete-based infrastructure and
the critical stage of concrete forming, thereby showing the prospects of CPCs in SHM.
Lu et al. [40] fabricated the CPCs sensor and analyzed its detection ability via acoustic
emission (AE). The results show that the embeddable sensor has a good detective perfor-
mance due to the reduction of external interference and improved ability to detect the AE
signals induced by the micro-cracks or dislocation. Another property of this composite
is the broadband characteristic, which can help analyze the loading process via AE fre-
quency content variation [29,114]. These advantages of the composite are also presented
in the case studies showing in Table 7. Dynamic mechanical monitoring can also be car-
ried out based on this composite. Dong et al. [66] monitored the mechanical–electrical
response of the composite, reporting that the electrical output signal could reproduce the
mechanical input signal with quite a complex waveform and frequency range without
any visible distortion. It holds a good performance to the dynamic mechanical signals
input directly in beam, frame, and transporting simulation tests and exhibits excellent
application potential in civil engineering. Considering the durability and stability of the
CPCs sensor, Wang et al. [115] investigated the location of the composite element in the
Sensors 2021, 21, 3230 23 of 29

sensor and characterized its mechanical–electrical responses in various conditions. The

results showed that the sensor possessed excellent linear performance when the ratio of
cement to epoxy resin was 3:1 and the sensing element was put in a position near the
underside of the encapsulation material; the fatigue load and water had a negligible effect
on its linearity and sensitivity, and in the intended temperature range (0~40 ◦ C), the sensor
showed good linearity, almost independent of temperature. Recently, based on the d33
(99 pC/N) improvement, Pan et al. [31] embedded the cement-based sensor in a mortar
specimen to detect its compressive strength growth via the EMI technique and compared
with a PZT sensor, reporting that a more sensitive distinction was observed in the electrical
impedance before and after it was embedded. Moreover, its effective monitoring frequency
is more easily obtained during the mortar strength monitoring, which is beneficial for
evaluating the change in the material properties in SHM with higher accuracy.

Table 7. Application of cement-based piezoelectric ceramic composites.

Techniques Objects Achievements References

 Small nonlinear piezoelectric
effect with minimal impact.
 Excellent performance in
• Dynamic mechanical
characterizing dynamic signals.
Mechanical–electric evaluation Dong et al., 2011 [66]
 Excellent electrical output signal
response
repeats the complex mechanical
input signal.
 Rapid response to load.
 Excellent load transmission
• Sensor performance relates to the position of CPCs in
characterization the sensor. Wang et al., 2014 [115]
 Better sensitivity in higher
temperature.
 In-built cement-based sensor
• Investigate AE signals
avoids the distortion of AE.
detect ability of the
 Cement-based piezoelectric Lu et al., 2008 [40]; 2010
sensor
Acoustic composite with broadband [116]; 2011 [117]; 2011
• Crack detection
emission technique properties can efficiently monitor [29,114]; 2012 [118]; 2013
• Corrosion process of
the concrete structure [65]; 2016 [119]
reinforced concrete beam
deterioration.
 The active acoustic monitoring
method based on the in-built
cement-based piezoelectric
• Hydration process Lu et al., 2013 [30]; 2014
Ultrasonic technique composite is efficient to monitor
the growth of solid phases in [120]
concrete.
 In-built cement-based
piezoelectric composite has the
capacity to monitor the strength
• Strength development of evaluation.
Electromechanical the mortar  Cement-based piezoelectric Pan et al., 2020 [31]
impedance (EMI) composite is easy to find an
effective monitoring frequency
due to broader frequency
bandwidth.

6.2. Further Application

Generally, the SHM system is expected to operate stably and continuously under the
service environment. A cement-based piezoelectric ceramic composite sensor with superior
durability can be embedded in concrete, thereby mitigating environmental interference.
Due to the broadband property and excellent durability, the CPCs sensing element is
Sensors 2021, 21, 3230 24 of 29

expected to achieve long-term and large-scale monitoring in infrastructure. Addition-

ally, considering the many advantages of the cement-based piezoelectric composite, the
integrated multifunctional application deserves to be investigated. Sustainability is the
requirement for infrastructure. The energy-harvesting system has become a strategic object
and is expected to be combined with piezoelectric materials. Based on the principle of
electromechanical conversion, this composite could also be an energy harvester [79] that
collects energy under stable operation and act as an energy source in the power-off state.

7. Conclusions
Structural health monitoring (SHM) is the essential item for infrastructure to guaran-
tee the safety and responsibility of sustainability and economic efficiency. CPCs, durable
materials with compatibility for concrete, potentially achieve the sustainable and compat-
ible SHM, but some issues still exist in its materials design and fabrication process. The
profound understanding of CPCs can inspire systemic design and fabrication and expand
its application in concrete-based infrastructures. This paper performs a comprehensive
literature review on cement-based piezoelectric composites, including theories and ex-
periments analysis, materials, the preparation process, and application. The following
conclusions are summarized:

7.1. In Terms of Theories, Experimental and Simulation Study

Theoretical research for piezoelectric materials can promote understanding the ad-
vantage and working process of cement-based piezoelectric composites. The two-phase
model can also clearly describe the action process between the matrix and piezoelectric
particles. The imperfect surface and mechanical properties mismatch between the matrix
and function phase will significantly affect the piezoelectric performance. In terms of
experimental methods, the microstructure and piezoelectric performance are the essential
items in characterization. Investigation on the mechanical property has attracted increasing
attention, attributed to the insufficient stress transfer between the matrix and piezoelectric
ceramic particles. More mechanical properties parameters of CPCs after polarization need
to be further investigated, which help conduct performance prediction by combining with
the simulation.

7.2. In Terms of Materials

The factors considered for the three components are different. For ceramic: (i) content,
(ii) particle size, (iii) shape, (iv) lead-based/lead-free ceramics, and (v) particle surface,
can be considered to optimize the composite performance. For matrix, it is essential to
consider the properties, including (i) component, (ii) hydration product/hydration rate,
(iii) density, and (iv) dielectric properties. For admixture, the consideration of improving
(i) conductivity, (ii) density, and (iii) mechanical performance of the composite should
be carried out. Lead-based/lead-free piezoelectric ceramic can be the function phase
for the composite. Innovative cement materials are becoming more readily available.
More innovative cementitious materials are worth using as the matrix for CPCs, thereby
promoting the performance breakthrough and assisting in the highly efficient preparation
process. The admixtures could cooperate with cement to obtain a denser matrix and
enhance the matrix conductivity, which deserves further research.

7.3. In Terms of Fabrication Process

The fabrication optimization can achieve based on the properties of CPCs, especially
the cementitious materials, due to the conflicts between the cement matrix and piezoelectric
materials. The attention on the matrix performance improvement is valuable. Porosity and
moisture in the matrix are the major factors contributing to the polarization inefficiency
and breakdown. The temperature should be mainly determined based on the matrix and
ceramic type; polarization time can be considered according to the content and size of
ceramic particles; the electric field should endow the ceramics with higher performance
Sensors 2021, 21, 3230 25 of 29

and the matrix from breakdown. The application of intelligent manufacturing in the sensor
fabrication process is worthy of attention.

7.4. In Terms of Application

The embeddable cement-based piezoelectric sensor has been employed to monitor
the process, including cracking, steel corrosion, hydration, and strength development.
Compared with traditional piezoelectric sensors, the lower d33 still restrict the application
of CPCs. Realizing the long-term and large-scale infrastructural health monitoring based
on multi-functionalization is one of the strategies of this piezoelectric composite. The CPCs
with the ability to harvest energy are a potential application to achieve self-power.

Author Contributions: Conceptualization, W.D., Y.L., T.S., Q.W., N.H. and F.X.; methodology, W.D.,
Y.L., T.S.,Q.W., N.H. and F.X.; validation, W.D., Y.L.; formal analysis, W.D., Y.L.; investigation,
W.D., Y.L.; writing—original draft preparation, W.D., Y.L.; writing—review and editing, W.D., Y.L.,
T.S.,Q.W., N.H. and F.X.; supervision, Y.L.,T.S., Q.W. and F.X.; project administration, Y.L.; funding
acquisition, T.S. All authors have read and agreed to the published version of the manuscript.
Funding: This work was supported by JSPS KAKENHI Grant Number 19F19747, and the China
Scholarship Council (CSC NO. 202008440627, Joint-training PhD project).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The data presented in this study are available on request from the
corresponding author.
Conflicts of Interest: The authors declare no conflict of interest.

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