Additive Manufacturing of Piezoelectric Materials

Review
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Additive Manufacturing of Piezoelectric Materials

Cheng Chen, Xi Wang, Yan Wang, Dandan Yang, Fangyi Yao, Wenxiong Zhang,
Bo Wang, Galhenage Asha Sewvandi, Desuo Yang,* and Dengwei Hu*
efficiency and reduced the size of equip-

Additive manufacturing technology has attracted unprecedented attention ment, leading to technological progress in
in industry because it provides infinite possibilities for rapid prototyping and the development of small electronics. The
enormous potential and opportunities for the production of electronic devices development of these microminiatures,
of various complex shapes. This paper focuses on the progress of additive low power consumption, and portable
devices requires the continuous improve-
manufacturing of piezoelectric materials in recent years, summarizing the ment of battery energy density. However,
advantages of additive manufacturing technology and its technical impact traditional batteries have the limitations of
on the production of piezoelectric materials. It identifies the likely future short life, limited energy storage capacity
research development direction of additive manufacturing technology, as and low efficiency. Therefore, collecting
well as the limitations of the current additive manufacturing technology in energy from the surrounding environment
to power electronic devices to extend their
the context of piezoelectric materials. First, the various processes involved
service life and developing self-powered
in additive manufacturing of piezoelectric devices and the impact of various devices that do not require power supply
processes on device performance are systematically summarized. Then, replacement have become the focus of
the development of additive manufacturing technology and slurry prepara- research by many experts.[1–3] In addi-
tion of piezoelectric ceramic materials, piezoelectric polymer materials, and tion, the arrival of the Internet of Things
piezoelectric composites are introduced. Finally, the technical difficulties (IoT) has accelerated the development
of urban intelligence. The data capture,
and potential research directions associated with additive manufacturing data collection, and remote monitoring
of piezoelectric materials are discussed. With the continuous development of everyday items such as mobile phones,
of additive manufacturing technology and piezoelectric materials, additive laptop computers, medical technology,
manufacturing of piezoelectric devices with excellent performance, high and other electronic devices all need to be
energy storage density, and high electromechanical conversion efficiency will connected. The normal operation of sen-
sors requires energy consumption. If the
be applied in a wider range of fields in the future.
IoT is fully implemented, the number of
sensors will inevitably increase. When the
number of sensors increases to hundreds of millions, energy
1. Introduction
consumption will also increase, and the problem of environ-
The rapid development of artificial intelligence and mobile mental pollution will be unavoidable. If the energy of the envi-
electronic technology has prompted the continuous improve- ronment or the body can be captured to power these sensors, it
ment of semiconductor manufacturing technology and the con- will be a very beneficial method, as this power supply method
tinuous expansion of functionality, which has improved energy requires less maintenance, reducing the cost of subsequent
C. Chen, X. Wang, Y. Wang, D. Yang, Prof. D. Yang, Prof. D. Hu Dr. W. Zhang

Faculty of Chemistry and Chemical Engineering Institute for Solid State Physics
Engineering Research Center of Advanced Ferroelectric The University of Tokyo
Functional Materials Koto, Sayo, Hyogo 679-5148, Japan
Key Laboratory of Phytochemistry of Shaanxi Province B. Wang
Baoji University of Arts and Sciences State Key Laboratory for Mechanical Behavior of Materials
1 Hi-Tech Avenue, Baoji, Shaanxi 721013, P. R. China School of Materials Science and Engineering
E-mail: dsyang@bjwlxy.edu.cn, yangdesuo@163.com; Xi’an Jiaotong University
dwhu@bjwlxy.edu.cn, hdwpolymer@yahoo.co.jp Xi’an 710049, China
F. Yao Dr. G. A. Sewvandi
Department of Advanced Materials Science Department of Materials Science and Engineering
Faculty of Engineering and Design Faculty of Engineering
Kagawa University University of Moratuwa
2217-20 Hayashi-cho, Takamatsu 761-0396, Japan Katubedda, Moratuwa 10400, Sri Lanka
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202005141.
DOI: 10.1002/adfm.202005141
Adv. Funct. Mater. 2020, 2005141 2005141 (1 of 29) © 2020 Wiley-VCH GmbH
www.advancedsciencenews.com www.afm-journal.de
Figure 1. Additive versus subtractive manufacturing. a) In subtractive manufacturing, a block of material is processed by material-removing machines
according to digital design before obtaining the final 3D object together with a large amount of residual material. b) In additive manufacturing, a
starting material is processed by a 3D-printing machine, which deposits just the required amount of material in a layer-by-layer fashion before the final
3D object is obtained. Reproduced with permission.[65] Copyright 2016, Royal Society of Chemistry.
manual maintenance.[4–6] The development of energy har- and near-surface area depolarization of piezoelectric element,
vesting devices can not only effectively extend the service life of which results in the deterioration of the piezoelectric element
electronic equipment, but also bring convenience to equipment (Figure 1a).[28] Therefore, the use of traditional methods to fab-
with power supplies that cannot be changed easily. Although ricate complex and high-precision piezoelectric devices still faces
the existing green energy sources can provide power to elec- huge technical difficulties and product moulding risks. The rise
tronic devices efficiently, it is difficult to apply them to micro of additive manufacturing technology has ushered in the dawn
and small electronic devices with power on the order of mW of the development of new piezoelectric materials.
or µW because of their demanding use conditions and large Additive manufacturing including 3D printing (3D printing)
power generation. For these reasons, the energy generated by and 4D printing (4D printing) technologies, refers to fabri-
mechanical vibration and human movement has become a pop- cate complex 3D objects via digitally controlled deposition of
ular energy choice for microelectronic devices.[7–10] phase change and reactive materials and solvent-based inks.
At present, there are several ways to convert the mechanical It generally begins with the design of a 3D virtual model that
energy generated by vibration or moving objects into the elec- is sliced into several 2D horizontal cross-sections using a spe-
trical energy required by electronic equipment, including elec- cial software. By successively printing new 2D layers on top of
tromagnetic,[11,12] electrostatic,[13,14] and piezoelectric effect.[15,16] previous layers, a coherent 3D object can be finally fabricated
Compared with electromagnetic and electrostatic techniques, (Figure 1b).[29,30] Furthermore, 4D printed structures driven
piezoelectric materials stand out because of their high energy by electricity, magnetism, pH, solvent, light, shape memory
conversion efficiency and strong piezoelectric sensitivity.[17,18] materials, and biological signals have also appeared and exhib-
They can directly convert the applied mechanical stress into ited the new property and functionality besides the shape
available electrical energy and are easy to integrate into the changes.[31,32] The first commercial printer based on stereo-
system, thus attracting extensive attention. These materials lithography (SLA), developed by Charles Hull in 1986, opened
have been applied in many fields such as piezoelectric sen- the door to additive manufacturing.[33,34] To satisfy the demands
sors,[19,20] actuators,[21,22] ultrasonic transducers,[23,24] and energy of scientific research and product design, researchers have sub-
harvesters.[25,26] From this, we can see that piezoelectric mate- sequently developed the laminated object manufacturing,[35,36]
rials show great development potential for emerging func- fused deposition method (FDM),[37,38] selective laser sintering
tional materials and have become the focus of future research (SLS),[39,40] 3D printing (3DP),[41,42] etc. With the continuous
regarding renewable clean energy and advanced energy storage improvement of additive manufacturing technology, the tech-
materials.[27] nology has matured and gradually entered the mainstream
The traditional piezoelectric device is fabricated by subtrac- market.[43] Additive manufacturing technology has the advan-
tive manufacturing. This process is not only complicated, long tages of high material utilization rate, a rich material system,
production cycle, low utilization rate of materials, high manufac- high production precision, and the absence of shape structure
turing cost, but it also mainly employs cutting technology such as restrictions.[34,44] The ink it consumes includes a wide range of
scribing, broaching, sawing, or etching for piezoelectric devices ceramics,[45–47] metals,[48–50] and polymers.[51–53] Additive
with complex geometric shapes, which greatly limits operating manufacturing technology is widely applied in fields such as:
conditions, density and work surroundings of piezoelectric medicine,[54,55] robotics,[56,57] aerospace,[58] nanodevices,[59,60]
devices. In addition, the mechanical stress generated by the porous materials,[61] and many other fields,[62–64] because of its
traditional process will cause grain loss, strength degradation, uniqueness.
Figure 2. a) Trend of development for 3D printing. (Source: SmarTech).[68] b) Number of papers related to additive manufacturing piezoelectric mate-
rials over the past decade (2011–2019). Dates are from Web of Science. TS = (3D additive manufacturing OR 3D printing OR additive manufacturing)
and piezoelectric materials.
New paths for the manufacture of devices, multifunctional packaging steps;[75] and 5) improved electromechanical response
materials, and the complex design and manufacture of func- from 3D design, enhanced piezoelectric output, and increase
tional devices have been explored providing a wide range of device sensitivity.[75] Based on these advantages, additive manu-
application prospects, which is the trend and direction of future facturing technology has effectively promoted the development
development in various fields.[66] Figure 2a shows the growth of piezoelectric materials. Many experts and scholars are com-
of additive manufacturing technology since 2014 and the fore- mitted to research in this field and have made breakthrough
cast of the development trend of additive manufacturing tech- progress, and the number of relevant articles is increasing
nology. From 2014 to 2027, the growth is predicted to grow by (Figure 2b). However, there are still some urgent problems to be
10 times, particularly around 2025, which is about 2.4 times the solved in the development process. 1) Additive manufacturing
current (2020), showing an “explosive” growth trend. Additive technology adopts the process of “layered manufacturing, layer
manufacturing technology will bring huge economic changes by layer.” As the printing height and speed increase, the tight-
to the manufacturing industry, and the manufacturing industry ness between the layers is weakened, which can cause the
will also undergo major technological innovation. In the future, printing difficulty, and the low accuracy and the weak strength
there will be a wave of “hot” additive manufacturing. With con- of the printed parts. This cannot be compared with traditional
tinuous innovation, a new round of science and technology and technology. If some object models are peculiar, their positions
industries are creating historic opportunities, and there is great may require supporting structures, which can naturally increase
potential to transform traditional industries with new tech- the printing difficulty. 2) Although some piezoelectric materials
nologies. Additive manufacturing technology will completely have achieved a certain level of development in additive manu-
change the method of human production and will become the facturing, the technology overall is not very mature. It is still
symbol of the “Third Industrial Revolution.”[43,67] necessary to discover materials that can be used, and process
In recent years, additive manufacturing technology has been and materials must proceed in parallel to promote the contin-
primarily concentrated in the field of energy, such as the manu- uous innovation and breakthrough of piezoelectric materials.
facture of batteries, capacitors, piezoelectric devices, and other 3) The later manufacturing processes associated with the addi-
electronic devices,[69–71] because it can provide efficient and tive manufacturing of piezoelectric devices are complicated. If
convenient ways to fabricate electronic devices. Compared with the piezoelectric device can be directly integrated with other
traditional methods, additive manufacturing of piezoelectric components, the assembly and packaging steps of the device
devices has the following characteristics: 1) the ability to manu- can be eliminated, and the tedious subsequent processes can
facture the required complex structure;[72] 2) accurate control the be reduced, which will improve the manufacturing efficiency of
thickness and precision of the structure, with precise control the devices. These problems hinder the development of additive
for microminiature devices;[73] 3) by programming 3D active manufacturing of piezoelectric devices, and solving key tech-
topology, arbitrary piezoelectric constants can be combined;[74] nical problems will be the focus of future research.
4) direct integration of piezoelectric materials and other elec- Additive manufacturing technology provides a novel tech-
tronic devices eliminates the possibility of device assembly and nique for the rapid development of 3D functional piezoelectric
We focus on SLA, SLS, solvent evaporation-assisted 3D printing

(SEA-3DP), near-field electrospinning (NFES), FDM, electrical
poling-assisted additive manufacturing (EPAM), direct ink
writing (DIW), extrusion free forming (EFF), binder jetting (BJ),
and the advantages and disadvantages of these techniques for
making piezoelectric devices. These methods are classified in
three ways: point, line, and plane (Figure 4). The additive manu-
facturing is achieved by means of point-by-point into line, line-
by-line into plane, and plane-by-plane into a 3D part.[76] Figure 4
demonstrates the classification of additive manufacturing
processes used for the fabrication of piezoelectric materials
according to the dimensional order, the type of layer formation,
and the state of aggregation of starting materials.[45,77] Among
the dimensional order is based on the distinct deposition and
discharging ways of raw materials. For example, FDM usu-
ally is the starting materials with wires, and the continuously
extruded molten wire forms a 3D object in line-by-line and then
plane-by-plane manner.[32] DIW is the starting materials with
inks, and the ink jets in point-by-point first, and then line-by-
line and plane-by-plane manners finally.[78] SLS is the starting
materials with powders, and the powder is tiled on a printing
platform in plane way and sintered by laser. Furthermore, SLS
Figure 3. Main contents of this article: additive manufacturing, piezo-
deposits in plane-by-plane and then a 3D structure is fabri-
electric materials and additive manufacturing of piezoelectric devices. cated. SLA is similar to that of SLS and based on the ultraviolet
The major additive manufacturing technologies for piezoelectric mate- point light source, but it discharges is in the way of plane.[79,80]
rials include stereolithography (SLA),[79] selective laser sintering (SLS),[79] Digital light processing (DLP) deposits in plane-by-plane
fused deposition modeling (FDM),[79] direct ink writing (DIW),[79] electric manner according to the discharge way. Thus, DLP is classified
poling-assisted additive manufacturing (EPAM), reproduced with per- into the dimensional order of plane.[80] The purpose of the clas-
mission.[81] Copyright 2014, IOP Publishing, solvent evaporation-assisted
sification not only makes diverse printing method characteris-
3D printing (SEA-3DP), reproduced with permission.[82] Copyright 2014,
American Chemical Society, printed piezoelectric materials including tics distinct, but also is beneficial to understand how to fabricate
polyvinylidene fluoride (PVDF),[83] BaTiO3 (BT), reproduced with permis- the 3D structure from the starting materials to the discharge
sion.[83] Copyright 2020, Royal Society of Chemistry, PZT (Pb(ZrxTi1-x)O3), ways with the different printing processes. The deposition man-
reproduced with permission.[84] Copyright 2018, AIP Publishing LLC, ners can affect the bonding force between the fabrication layers,
and BaTiO3 nanowires (BT NWs), reproduced with permission.[82] Copy- resulting in poor precision, low density, and weak mechanical
right 2014, American Chemical Society, and printed piezoelectric devices
properties, which further weaken the piezoelectric properties
including transducers, reproduced with permission.[85] Copyright 2019,
Elsevier B.V. Reproduced with permission.[86] Copyright 2014, American of the device. Therefore, to select a process, the nature of the
Chemical Society. Reproduced with permission.[87] Copyright 2016, Else- material, the shape and size of the device, and the conditions
vier B.V., ultrasonic arrays, reproduced with permission.[88] Copyright and function of the device need to be considered. In addition
2019, MDPI Journals, nanogenerators (NG), reproduced with permis- to the deposition method, the working principle, printing pro-
sion[89] Copyright 2017, Elsevier B.V., and sensors, reproduced with per- cess, and advantages and limitations of various methods are
mission.[90] Copyright 2017, Springer Nature Ltd. discussed. The effects of piezoelectric materials applied in
additive manufacturing technology and the mixing process of
devices with complex structures and excellent performance. dopant and slurry on the performance of piezoelectric materials
This article provides a comprehensive review of the progress have been studied. The results reveal the potential development
made in additive manufacturing of piezoelectric devices and opportunities of additive manufacturing of piezoelectric devices
the development of printable piezoelectric materials (Figure 3). and point out the direction for future development.
Figure 4. Additive manufacturing processes classified by the printing process and type of layer formation.
Table 1. Summary and comparison of the additive manufacturing of piezoelectric devices with various methods and materials.
Printing method Materials Printing size [mm] d33 [pC N−1] εr Electric field for poling
SLA KNN [85]
D=8 170 2150 3 kV cm−1, 30 min
PZT [91]
15 × 15 × 3 212–345 760–1390 30–40 kV cm−1, 70 °C, 15 min
BT[87] D = 10 160 1350 30 kV cm−1, 100 °C, 30 min
BT [86]
0.25 × 0.25 × 0.1 40 – 12 mV m−1, 120 °C, 24 h
BT[88] 12 × 3 166 2177 30 kV cm−1, 15 min, 70 °C
BT[92] D = 10 87 920 2 V µm−1, 120 °C, 30 min
PVDF [93]
30 × 5 × 1 – – 3 mV m−1, 15 h
PMNT[94] 18 × 32 620 – 1 kV mm−1, room Temp., 1 min
Acrylate [95]
140 × 100 × 20 – – 2400 V m−1
BJ BT [96]
12 × 12 × 3 74.1 – 2 kV cm−1, 120 °C
EFF PNN–PZT[97] D=3 – – –
BT [98] – 200 2200 5.4 kV cm−1, 90 °C, 12 h
FDM PVDF[99] 10 × 25 × 0.65 5.8 × 10−2 – 12 kV
PVDF[100] 60 × 10 d31 = 1.19 pm V−1 – 8.33 mV m−1, 80 °C
BT + PVDF [101]
11.5 × 37 × 0.33 d31 = 0.021 – 35 mV m−1, 90 °C, 2 h
PVDF + BT[102] 30 × 11 – – –
BT + ABS[103] 24.6 × 15.2 × 15.5 cm 8.72 – –
SLS PZT[104] 10.1 × 10.1 × 3.5 – – 0.54 kV mm−1, 70 °C, 2 h
BT[105] – 2.1 – 80 °C, 15 min
DIW PLZT[106] – 481 1986 3.5 kV cm−1, 120 °C, 20 min
5 kV cm−1, 120 °C, 20 min
BT[89] – – – 30–200 kV cm−1, 3 h
EPAM BT + PVDF[107] 7.5 × 40 – – 40 mV m−1
PVDF [81]
100 × 50 – – 2 mV m−1
NFES PVDF[90] 40 × 20 × 2 – – –
SEA-3DP BT [108]
10 × 45 × 100 µm – – 10 mV m−1, 90 °C, 12 h
PVDF[82] 30 × 30 – – 1 mV m−1
PVDF[75] 20 × 5 × 0.1 – – –
2. Additive Manufacturing Process steps for the piezoelectric devices, and reduce the manufac-
for Piezoelectric Devices turing costs and control the porosity and the precision of the
devices. In Table 2, the advantages and disadvantages of the
As an emerging and cutting-edge manufacturing method, various additive manufacturing methods are comprehensively
additive manufacturing technology promotes the development compared. The extrusion-based methods usually discharge
of piezoelectric devices, from one-step moulding of micro- directly from the nozzle into the dispenser deposition model
miniature to large-scale devices, to improve the performance after material pretreatment or employ self-supporting materials
of piezoelectric devices. Table 1 lists the materials, sizes, and to create objects. This method has gained widespread appli-
performances of typical additive manufacturing of piezoelectric cation because of its simplicity and low manufacturing cost.
devices by various methods and materials and polariza- Although its creation process is independent, it still needs to
tion conditions. It can be found from Table 1 that compared be postprocessed to harden it and improve its mechanical
with traditional methods, the performance of the printing properties through drying, heating, or sintering steps. Photo
piezoelectric devices is weak and still needs to be improved. polymerization cures each layer by exposing the liquid polymer
Moreover, the available materials are limited, which limits the to ultraviolet light, stacking layer by layer, and demonstrates
widespread application of additive manufacturing in the field good adhesion between each layer. For complex designs, self-
of piezoelectric materials. Although the application of addi- supporting materials are still required to make the printed
tive manufacturing in the field of piezoelectric materials has structure independent. Powder-based methods use solid parti-
certain limitations, it is worth noting that additive manufac- cles to build a layer structure. The powder is distributed on the
turing technology can control the size and shape of the device. surface of the object, scraped into a thin layer, and after the first
There are no restrictions on working conditions and application layer is cured, the second layer can be deposited. The advan-
environments, and it can greatly simplify the manufacturing tage of such technology is that the remaining powder in each
Table 2. Comparison of additive manufacturing techniques for piezoelectric devices[65,79,109].
Process AM method Available materials Advantage Limitation Applications

Polymerization SLA Photocurable resins, Simple operation method, high Not suitable for multimaterial Rapid tooling patterns, snap
photopolymers, ceramic, resolution, mixing, high slurry fits, very detailed parts,
metal or high surface precision, requirements, not suitable for presentation models, high heat
polymer particles in the resin high efficiency the preparation of large devices applications
Extrusion EFF Polymer, sol–gel Simple operation method, no Low density, low surface finish, Rapid mass production of large
need to demould, Not easily unable to prepare microdevices devices, making of simple food
deformed, no mask required applications
Extrusion FDM Thermoplastic, polymers, User-friendly, low cost, large Weak mechanical properties, Small detailed parts, presenta-
polymer-based size capabilities, wide range of high viscosity of the molten tion models, patient and
nanocomposites applications materials, low surface quality food applications, high heat
applications
Extrusion DIW Thermoplastics, sol–gel, Affordable cost, easy Weak mechanical properties, Very detailed parts, rapid
metal, ceramics operation, large material diver- high ink requirements tooling
sity, and no mask requirement patterns, jewelry and fine items
Powder-based SLS Thermoplastics, metal Bulk objects from various Material surface fineness, low Less detailed parts, parts with
powdered materials, no mould surface quality, low resolution snap-fits and living hinges, high
required, low cost heat applications
Powder-based NFES Ceramics, polymer, Increase piezoelectric output, Weak mechanical properties, Making free-form piezoelectric
composite simple, economical and complicated subsequent devices, production of bulk
versatile operations materials
Powder-based EPAM Piezoelectric polymer Good uniformity in production Weak mechanical properties, Making free-form piezoelectric
material, piezoelectric and simple fabrication step, low high ink requirements devices,
ceramic material cost, single processing suitable for sensing, actuation
with simplicity
Solvent-based SEA-3DP Polymer, composite Scalable, rapid, versatile, high High material requirements, Suitable for small, simple
efficiency, simplicity, versatility, not good for high volume structures, making free-form
and controllability printing, and print head is less piezoelectric devices
durable
layer can be used as a self-supporting material without the need The film coated with 15 µm of BT ink showed no cracks, dem-
for additional materials, thereby reducing material waste. The onstrating a highly dense ceramic on a flexible substrate mem-
solvent-based methods deposit the solvent on the substrate brane. To improve the piezoelectric output performance, the
through the nozzle. After the evaporation of one layer of solvent fabricated film was polarized under a strong electric field of
is completed and the material is solidified, the next layer can be 30–200 kV cm−1 for 3 h. Then, physical simulation and piezo-
deposited. None of the layers requires a self-supporting struc- electric potential distribution calculation regarding the BT film
ture, and the method is easy to operate. However, it is only suit- were performed. As shown in Figure 5b, the BT mixed film, with
able for the production of simple structures. At present, there an effective area of 3 cm × 4 cm f-PEH was bent at a radius of
are still many urgently challenging problems to be solved in the 0.74 cm, or 3.54%. When deformed at a strain rate of 0.236%, the
additive manufacturing of piezoelectric devices. This section resulting open-circuit voltage (Voc) (Figure 5c) and short-circuit
mainly summarizes the piezoelectric devices made by advanced current (Isc) (Figure 5d) reached 7.0 V and 2.8 µA, respectively.
additive manufacturing technology in recent years and briefly When the resistance was 2 MΩ, the maximum instantaneous
discusses the advantages and disadvantages of the various pro- power on the load resistor was 5 µW. This method provides an
cess methods. innovative platform for self-powered flexible electronic devices.
To improve the piezoelectric performance of the material, a
DIW process was used to prepare oriented flexible nanocom-
2.1. Point to Line-Based Method posite capacitors (Figure 5e).[110] A nozzle with a diameter of
100 µm was used to create a high-shear environment and pro-
2.1.1. Direct Ink Writing mote anisotropic nanocomposites to obtain BaTiO3 nanowires
(BT NWs) arranged in parallel by shear stress induction. By
DIW is a droplet-based deposition technology in which mate- testing the characteristic breakdown strength of nanocompos-
rial is directly deposited on the substrate through a nozzle. By ites with oriented and random structures under different loads,
controlling the deposition rate of droplets, devices with high it was found that nanocomposites with aligned BT NWs had
resolution and complex patterns can be produced. It has the higher breakdown strength at the same load level (Figure 5f).
advantages of low price, simple operation, and diverse avail- In addition, it can be seen from Figure 5g that the discharge
able materials.[79,89] An f-PEH-based BaTiO3 (BT) hybrid film energy density of the nanocomposite filled with BT NWs
shown in Figure 5a using a simple inkjet printing process.[89] increases with increasing load level at a high field. When the
Figure 5. a) A simplified simulation model for calculating the piezopotential distribution inside a piezoelectric BT film sandwiched between two
electrodes when horizontally subjected to tensile stress.[89] b) Calculated simulation results showing the piezoelectric potential introduced inside
a BT layer by bending with a bending radius of 0.74 cm.[89] c,d) Output voltage and current signals from an f-PEH in the forward (left) and reverse
(right) configuration with a measurement kit. Reproduced with permission.[89] Copyright 2017, Elsevier B.V. e) A nanocomposite capacitor for energy
storage applications.[110] f) Breakdown strength of P(VDF-CTFE) nanocomposites as a function of BaTiO3 loading.[110] g) Discharge energy density of
P(VDF-CTFE) nanocomposites filled with aligned BT nanowires. Reproduced with permission.[110] Copyright 2020, Royal Society of Chemistry. h) Optical
images of the different woodpile sizes.[112] i) SEM image of the KNN powders.[112] j) Hysteresis loop of the sintered KNN sample. Reproduced with
permission.[112] Copyright 2015, MDPI Journals.
loading was 5.0 vol%, the maximum energy density of the BT dicular to the direction of the electric field and compared with
NW oriented nanocomposites was 14.52 J cm−3, which was 55% random distribution. The dielectric constant of the nanocom-
higher than the maximum energy density of randomly oriented posite materials with regularly arranged BT NWs was smaller
BT NWs nanocomposites under the same conditions. Then, than the nanocomposite materials with random BT NWs.
the frequency-dependent dielectric constant of BT NWs/polyvi- With the advancement of the wearable electronics, the stretch-
nylidene fluoride-chlorotrifluoroethylene (P(VDF-CTFE)) nano- able energy harvesters are attractive to reduce the need of fre-
composites was tested, where BT NWs were arranged perpen- quent charging of wearable devices. A BaTiO3 nanoparticles
Figure 6. a) Schematic of the proposed process leading to increased β phase fraction in PVDF with filler addition.[75] b) Structures fabricated using
10 wt% BaTiO3 ball-milled nanocomposite solution. Reproduced with permission.[75] Copyright 2017, American Chemical Society. c) Comparison of
charge output test after five years.[82] d) Piezoelectric charge outputs of PVDF and NC sensors fabricated with different electric fields.[82] e) Schematic
of the sensors printed on a shoe insole (not to scale). Reproduced with permission.[82] Copyright 2018, American Chemical Society. f) Voltage signals
generated from BT nanocomposites.[108] g) Current signals generated from BT nanocomposites.[108] h) Generated peak power for the cast and printed
nanocomposites with 0°, 45°, and 90° fill angles. Reproduced with permission.[108] Copyright 2018, American Chemical Society.
(BT NPs)/P(VDF-TrFE) piezoelectric ink was used to make a dielectric constant was 1775, and the residual polarization ratio
stretchable piezoelectric nanogenerator with a kirigami struc- was 18.8 µC cm−2 (Figure 5j). The experimental data reveal that
ture by DIW.[111] A square thin film sample (an effective area the sintered sample had suitable electrical properties, and this
of 1 cm × 1 cm) was printed using ink filled with 20 wt% BT process did not require any mould, which simplifies the mate-
NPs, which can generate voltage of 6 V and current density of rial production process. This result provides a new idea for the
2 µA cm−2 by the applying force of 60 N at frequency of 5 Hz. design and application of new piezoelectric devices.
When the load resistance is 107 Ω, the maximum power density Overall, DIW is a relatively new piezoelectric device manu-
is 1.4 µW cm−2. This work further demonstrates that the poten- facturing process that has wide application potential in small-
tials of composite materials and DIW can improve the perfor- scale production. The DIW process has the advantages of a
mance of piezoelectric devices for the broad applications in the wide range of material applications, less material waste, and
medical implant and the neurological diseases. high resolution. The ink extrusion through the nozzle can
Moreover, a piezoelectric (K, Na) NbO3 (KNN) grating with improve its shear elastic modulus, tensile strength, and shear
a wood structure and a high piezoelectric constant was fabri- strength, which is conducive to maintaining the shape of the
cated by DIW using a methyl methacrylate ink (Figure 5h).[112] device and improving the mechanical properties of the devices
Figure 5i demonstrated that its micromorphology was highly while maintaining piezoelectric performance. Its main limita-
dense, and its relative density could reach 98% when sin- tions are low printing speed; high requirements regarding ink
tered at 1100 °C for 2 h. Under an electric field of 8.5 kV cm−1, formulations, nozzles that are not durable, easily blocked, and
the piezoelectric coefficient (d33) value was 280 pC N−1, the damaged; and its unsuitability for large-scale production.
2.1.2. Solvent Evaporation-Assisted 3D Printing a maximum power of 15.3 nW at 0.35% strain (Figure 6h). The
electromechanical performance indicated that the arrangement
SEA-3DP can deposit a highly volatile piezoelectric nanocom- of NWs had a significant effect on the energy harvesting per-
posite solution on the surface of an object through the nozzle. formance of nanocomposites. In embedded nanostructures, the
After the first layer evaporates and solidifies, the next layer can optimal power output can be increased by eight times. Com-
be deposited, and this process continues until the device is pared with the randomly oriented nanocrystals prepared by the
completed. The process is simple in operation and low in pro- traditional casting process, the power generation capacity can
duction cost.[82,108] Bodkhe et al. studied the role of BT NPs in be improved by 273%.
the formation of β polymorphs in 3D printable polyvinylidene The SEA-3DP process makes use of solvent evaporation to
fluoride (PVDF), and fabricated layered and self-supporting extrude the nozzle from a fluid state to a solid state, which is
piezoelectric structures on the scale of µm to mm using SEA- conducive to the maintenance of self-supporting shapes and
3DP (Figure 6b).[75] The experiment found that doping 10 wt% reduces the waste of self-supporting materials. It is usually used
BT in PVDF led to the best loading and average size, the best to make simple-shaped piezoelectric devices. However, there
crystallinity, and can effectively prevent PVDF from changing are still some limitations. In the process of relative movement
to the α phase, leading to significantly improved piezoelectric of the nozzle, uneven inkjets may appear, and the resolution in
output. By comparing different filling methods, the best pro- the x-axis direction is inconsistent, resulting in an unbalanced
cess for the preparation of BT-PVDF composite material was mechanical stress of the devices. In addition, the rheology and
determined to be the ball milling method. Adding BT NPs to volatility of the slurry is difficult to control, leading to the preci-
PVDF by ball milling helped increase the β phase nucleation sion of the device is low and the mechanical strength is poor.
sites on NPs, as a result of the strong O·H···FC hydrogen
interaction at the hydrogen atom (Figure 6a). Then, a cylin-
drical sensor was fabricated with 0.25 g mL−1 of a 10 wt% BT 2.1.3. Binder Jetting
NPs ball milled nanocomposite solution. When tapped lightly
with a finger five times, the sensor generated a maximum BJ technology has the advantages of simple operation method
voltage output of 4 V, and the voltage generated when it was and low cost, and it can be applied to the fabrication of devices
released was −2 V. The voltage generated by a 3D sensor is of any size.[96] In a previous experiment, the binder jetting tech-
approximately ten times higher than the voltage of a thin- nology was used to produce a BT sample (Figure 7a).[96] The den-
film sensor with the same electrode surface area. The team sity and crystal structure of the printed device were optimized by
continued to use the SEA-3DP process to fabricate PVDF-BT modifying the forming parameters (binder saturation and layer
nanocomposite thin-film sensors (Figure 6e).[82] It can be seen thickness) and sintering curve. The surface and cross-section
from Figure 6c that the addition of BT NPs can improve the morphology of the BT sample after sintering were characterized
sensor’s charge output, and under a polarization electric field of by SEM, and it was found that the local grains of the BT sample
1 MV m−1, the charge output increased by 300% compared with after sintering grew and the density increased (Figure 7b). The
the pure PVDF phase. Then, a sample was selected for testing dielectric constant frequency range of BT samples sintered at
after one year, and it was found that the charge output was 1260 °C was 12.4–18 GHz, determined using Ku-band waveguide
significantly decreased (Figure 6d), indicating that the sensor and vector network analyzer. For the samples sintered at 1400 °C,
produced by this process had poor stability, and the process the d33 value is 74.1. The dielectric constant at different tempera-
method still needed to be improved. The SEA-3DP process can ture (Figure 7f) and dielectric loss at different temperature with
precisely apply printing pressure, so it is suitable for printing 1 kHz were measured (Figure 7c). The findings showed that as
of oriented materials. Malakooti et al. applied the SEA-3DP pro- the sintering temperature increased, the dielectric constant also
cess for the alignment of functional nanowires in a polymer increased. The dielectric constant and dielectric loss at different
matrix.[108] The high-aspect ratio BT NWs was dispersed in a frequencies (Figure 7d,e) were low at 1330 °C.
polylactic acid (PLA) to produce a printable piezoelectric solu- The BJ process has the advantages of simple manufacturing
tion. By adjusting the arrangement of the nanowire filler in method, no material size limitation, and strong practicability,
the active nanocomposite, the electromechanical response was making it suitable for the manufacture of amorphous devices.
improved, thereby improving energy harvesting performance. However, because the weak resolution, the poor precision, and
BT-PLA nanocomposite samples prepared by this process can printing efficiency, and the uneven stress derived from the
clearly be observed as arranged BT NWs. The longitudinal axis nozzle occur, the mechanical strength and stability of the mate-
of the printed devices is the axis of interest, and the estimated rial can greatly reduce and the fracture can easily exist between
HOF values for 0°, 45°, and 90° infill angles were 0.455, 0.236, the layers, leading to the low piezoelectric performance. This
and 0.254, respectively, which were lower than the theoretical greatly limits the generalization of this method.
HOF values of ideally oriented high length-diameter fillers.
The voltage signal from the BT nanocomposite at 0.35% strain
and an excitation frequency of 5 Hz was tested. The short- 2.2. Line to Plane-Based Method
circuit current and voltage generated were highly dependent
on the printing direction of the nanocomposite and the applied 2.2.1. Fused Deposition Modeling
strain (Figure 6f,g). The nanocomposite with BT NWs arranged
in the load direction (0° printed nanocomposite) produced the In FDM, the material is extruded through a nozzle to track the
highest AC power over the entire range of load resistance, with cross-sectional geometry of the part layer by layer. The material
Figure 7. a) Schematic of binder jetting technology. b) Low-magnification image of BT specimen sintered at 1400 °C. c) Dielectric loss for BT at 1 kHz
at various temperatures. d) Dielectric constant for BT fabricated by BJ technology. e) Dielectric loss for BT fabricated by BJ technology. f) Dielectric
constant for BT at 1 kHz at various temperatures. Reproduced with permission.[96] Copyright 2015, Elsevier B.V.
is usually in the form of filaments. It has the advantages of low 1 Hz. Under these conditions, the d33 of the BT/PVDF nano-
cost, unlimited size, and a wide application range.[79]There are composite was 21 × 10−3 pC N−1, which is three times that of a
many factors that affect the formation of the PVDF β phase solvent cast nanocomposite.
when a PVDF film is prepared by FDM.[100] Figure 8c demon- In addition, the integrated process of the fused deposi-
strated the effect of different extrusion speeds on the formation tion and corona polarization (IPC) (Figure 8a) further sim-
of β phase. The printing speed affected the dipole alignment of plified the printing process and had become a popular new
the sample in the print bed and thus affecting generation method. Using IPC to make PVDF film, the test found that
of the β phase. As can be seen from Figure 8e, with a change the β phase content of the PVDF film at room temperature
in printing speed, the surface morphology underwent some was significantly higher than that at other temperatures.[99]
changes. After the printed sample is polarized, the d31 can reach As the temperature of the heating bed increases, the piezo-
1.19 pm V−1 and the Young’s modulus averaged 457 MPa. When electric effect of the PVDF film decreases significantly. When
the force was parallel to the extrusion path, Poisson’s ratio of the a voltage of 12 kV is applied during the IPC process, the
single-layer extrusion is the lowest. Figure 8d demonstrated PVDF film can generate piezoelectric output current reaching
the effect of in situ polarization on formation of the β phase. ±0.106 nA, the ultimate strength was increased from 17.0 to
An electric field applied to the PVDF increases the β phase con- 19.8 MPa, the strain was reduced from 45.4% to 38.6%, and
tent at elevated temperatures. In addition, the heated bed mate- the d33 value can reach 4.8 × 10−2 pC N−1. The piezoelectric
rial has an effect on formation of the β phase (Figure 8b). The constant increased linearly with increasing applied voltage.
use of FDM process can increase the β phase content, thereby This strategy provides an effective method for improving
optimizing the piezoelectric performance of the material, so it the piezoelectric property of PVDF. Furthermore, another
was widely applied. work is explored the best conditions for fabricating PVDF
In order to further enhance the piezoelectric properties of materials.[113] It was found that the extrusion temperature
PVDF, a BT-based PVDF nanocomposite was prepared to make of PVDF filaments should be selected within the range of
the piezoelectric devices by the FDM process.[101] First, through 200–230 °C and the heating bed temperature needs to be 90–110 °C.
filament extrusion process, the agglomeration of BT in PVDF In addition, the feasible extrusion speed range for printing PVDF
is reduced and the composite material was evenly dispersed. is 10–25 mm s−1, and the peripheral speed is kept below 20 mm s−1.
Then, the piezoelectric response of BT/PVDF nanocomposites Finally, according to a 95% confidence window, Young’s
was improved by thermal polarization. The current output of modulus and β phase fraction of PVDF printed samples with
the sample increases by five times after thermal polarization, 70% infill density were in the range of 772.46 ± 44.3 MPa and
and the total current output was increases by 500% compared 0.4336 ± 0.048, respectively. The FDM process has a great appli-
to with the value before thermal polarization (Figure 8f). cation potential in the polymer material fabrication. Moreover,
Figure 8g showed the application of 50 cyclic loads at 40 N and the technology can also be applied to make the electrets.[114]
Figure 8. a) Schematic of corona poling process. Reproduced with permission.[99] Copyright 2017, IOP Publishing. b) Effect of bed material on the
amount of PVDF β phase.[100] c) Effect of speed on the amount of PVDF β phase using the flat nozzle.[100] d) Effect of extrusion temperature on the
amount of PVDF β phase.[100] e) SEM images of the top surfaces corresponding to different feed rates. Reproduced with permission.[100] Copyright 2017,
Elsevier B.V. f) Current output of solvent-cast and printed 9 wt%-BT/PVDF film after thermal poling process.[101] g) Cyclic loadings at 1 Hz applied on
samples by fatigue machine. Reproduced with permission.[101] Copyright 2018, SAGE Journals.
The FDM process has become one of the most commonly allowing simultaneous printing and polarization to continu-
used additive manufacturing technologies and has been used in ously produce piezoelectric devices of any shape.[81,107] Additive
many fields. However, the raw material manufacturing process manufacturing of BT powder piezoelectric sensors can be filled
is complicated, and the doped material and the thermoplastic with PVDF substrates by in situ polarization (Figure 9a).[81]
material can only be used after being mixed, which increases When filled with 15 wt% BT, they demonstrate high surface
the complexity of the manufacturing process and the manu- density (Figure 9c), the PVDF β phase was 55.91% (Figure 9b),
facturing cycle. The high mixing processing temperature leads and the PVDF β phase and output current were increased by
to the thermal degradation of some dopants, which seriously 30.41% and 1033%, respectively (Figure 9g). The d33 value was
hinders the performance of piezoelectric composite devices. correspondingly increased by 0.101 pC N−1. The dynamic load
In addition, the resolution of the FDM process is usually low, fatigue strength of the composite material was tested. As can be
especially in the z-axis direction, the layers are easily deformed seen from Figure 9f, the ultimate tensile strength decreased as
and the gaps are large, resulting in poor surface quality, weak the content of BT increased. At 3 wt% BT, the ultimate tensile
mechanical properties and low electromechanical responsive- strength of the film increased by ≈45.83%. It decreased to 7.63%
ness. Therefore, it is not suitable for the manufacture of high at 15 wt% BT. With the BT loading increasing, the agglomera-
precision devices. Moreover, in the FDM process, the wire tion phenomenon and microcracks increased and the tensile
output can be uneven and rough, which seriously affects the strength decreased. To further test piezoelectric performance of
controllability and density of printing. PVDF materials, the effect of different electric field strengths
on the piezoelectric response of PVDF films fabricated by
the EPAM process was investigated.[107]When the electric
2.2.2. Electric Poling-Assisted Additive Manufacturing field strength was tested at 0.0, 1.0, 2.0, and 3.0 MV m−1, the
printing of the film was changed, the results indicated that
EPAM is a recently developed additive manufacturing process for samples without an electric field applied change occurred,
that combines electrical polarization with fused deposition, and the printing conditions were stable, with no abnormalities.
Figure 9. a) Schematic of the in situ additive manufacturing and dipole alignment of PVDF and BT filler.[81] b) β phase content for nonpoled printing
PVDF and poled printing PVDF/BT films with different BT contents.[81] c) SEM images of the surfaces of printing composite films with compositions
of 15 wt% BT/PVDF. Reproduced with permission.[81] Copyright 2014, IOP Publishing. d) Testing method of printed PVDF devices: testing board.[107] e)
Cu electrodes, cuplaced at both ends of the PVDF piezoelectric device. Reproduced with permission.[107] Copyright 2017, Wiley-VCH. f) Generalized
S–N curve for additive manufacturing PVDF/BT films with different BT contents.[81] g) Output currents of ABS, nonpoled PVDF, poled PVDF, and BT/
PVDF films with different BT contents under 40 N. Reproduced with permission.[81] Copyright 2014, IOP Publishing.
When the electric field strength was 3.0 MV m−1, the first sensitivity of the device and inferior electromechanical
film printed was broken, and it was difficult to maintain a responsivity.
stable electric field. Then, when the electric field strength was
2.0 MV m−1, the area of the fabricated PVDF polymer device
was 100 mm × 50 mm (Figure 9d). Next, the current test device 2.2.3. Near-Field Electrospinning
shown in Figure 9e was used to detect its manual bending and
release device, with an output current of ≈±1.5 nA. This work NFES is a method for accurately depositing 1D or 2D highly
demonstrates the potential of the EPAM process to improve the oriented micro/nanofibers (NMFs) by electrodeposition of
performance of flexible piezoelectric devices, which can be used polymer solutions.[90,115] A previous study adopted NFES to fab-
in sensing equipment and medical equipment. ricate a piezoelectric generator. The main steps of the manu-
Overall, the EPAM process combines the fast printing of facturing process are shown in Figure 10a.[90]According to the
the FDM process with electric polarization, which improves SEM image of electrospun fibers, the diameter of NMFs ranged
the fabrication efficiency of the device. However, the raw from 1 to 5 µm, the continuous deposition length was ≈35 mm,
material is limited to thermoplastic polymers generally and and the fiber pattern had the same period of ≈15 µm. Three
the adhesion between the printed layers is weak, resulting in types of device topologically self-powered sensors (WSS) with
the low mechanical properties of the printed parts. Moreover, the different topologies were fabricated, and the output current and
printing speed and resolution are low and the polarization field voltage were 50, 70, and 100 nA and 2, 3.5, and 3.5 V, respec-
strength is difficult to control, leading to the low piezoelectric tively (Figure 10d). WSS is an integrated device for self-powered
Figure 10. a) Piezoelectric generator with fibers of wavy and 3D topology demonstrated and the fabrication process, which consists of four main steps.
Reproduced with permission.[90] Copyright 2017, Nature Publishing Group. b) Conformation changes and specific interactions between PVDF and
PMLG fibers. Reproduced with permission.[115] Copyright 2015, Royal Society of Chemistry. c) Demonstration of the integration of WSS as a self-powered
foot pressure mapping sensor for detecting applied multiple forces in real time.[90] d) Schematic of the experimental setup and three topologically
different surfaces, output voltage, and current versus stretching–releasing deformation strain of 0.5% at 4 Hz. Reproduced with permission.[90]
Copyright 2017, Nature Publishing Group.
foot pressure mapping sensors that can detect multiple applied electrodes to capture a maximum voltage of 0.08 V, maximum
forces in real time. The average output voltage and current with power of 637.8 pW, output voltage of 0.019–0.185 V, and energy
amplitudes of 0.5, 1, and 1.5 mm were found to be 1, 1.5, and conversion efficiency of 3.3%. Compared with the original pro-
2 V and 60, 100, and 150 nA, respectively. As can be seen from cess, the energy efficiency was improved by three times. This
Figure 10c, WSS with an effective area of 4.5 cm × 3 cm was process can be applied to many fields, such as medical engi-
arranged on the electrodes in the matrix, and the different pres- neering, wearable sensors, and energy harvesting.
sures from the feet can directly measure the strain distribution In summary, the NFES process of electric deposition can
of WSS. The advantages of the NFES process are obvious in the improve the dipole orientation without additional processes.
fabrication of the PVDF materials. Pan et al. further adopted the The microstructure is controlled by the nozzle diameter, extru-
NFES process to produce a PVDF/poly (γ-methyl l-glutamate) sion pressure, extrusion temperature, and extrusion speed,
(PMLG) composite (Figure 10b) energy harvesting device.[115] so the controllability of the NFES process is quite excellent.
The combination of PVDF and PLMG increased the orientation However, the NFES process usually has low resolution, which
density of dipoles because of the intermolecular hydrogen affects the printing accuracy. Moreover, the low mechanical
bonding and improved the mechanical properties of the mate- strength associated with the bonding force between layers leads
rial. In addition, the NFES process was used to improve the to a decrease in mechanical strength of the device, which seri-
PVDF/PMLG composite and increase the dipole orientation, ously affects the piezoelectric performance and agility.
thereby effectively improving the piezoelectric performance of
the device. Microtensile testing determined that the high ulti-
mate stress of the composite was 24.47 MPa and the Young’s 2.2.4. Extrusion Free Forming
modulus was 2.77 GPa. The PVDF/PMLG energy collection
device was fabricated by pressing the piezoelectric composite Extrusion free forming method is to deposit a paste layer by
fiber membrane to a poly(ethylene terephthalate) with parallel layer through a nozzle to form a 3D object. This process is
Figure 11. a) Configuration of the extrusion system.[97] b) Microstructure of the fibers after sintering at 1200 °C (with the sol to powder ratio 1:7). Repro-
duced with permission.[97] Copyright 2004, SAGE Journals. c) High-magnification SEM image of sample sintered at 1400 °C.[98] d) 3D printed sample
(right) and shrunk sample after sintering and polishing processes (left). The inset shows a side view of the green body. Reproduced with permission.[98]
Copyright 2019, Wiley-VCH. e) Cross-section of a dried green fiber with a sol to powder ratio of 1:7. Reproduced with permission.[97] Copyright 2004,
SAGE Journals. f) Dielectric constant (εr) respectively as a function of frequency from 101 to 106 Hz for samples sintered at 1100, 1200, 1300, and
1400 °C. Reproduced with permission.[98] Copyright 2019, Wiley-VCH. g) Ferroelectric properties of the fiber composites.[97] h) Piezoelectric properties
of the fiber composites. Reproduced with permission.[97] Copyright 2004, SAGE Journals.
usually used to produce piezoelectric devices with simple suggests that the sintered samples have high density.
geometric shapes and has the advantages of low produc- Based on the experimental data, when the BT content was
tion costs and no adverse environmental conditions.[97,98] In 35.45 vol% (77.01 wt%). The density of the printed BT ceramic
a previous study, slurry extrusion (Figure 11a) was used to was 3.93 g cm−3 (65.3%), reaching its maximum value. At
prepare Pb(Nb, Ni)O3–Pb(Zr, Ti)O3 (PNN-PZT) by adjusting 103 Hz, the piezoelectric and dielectric properties were found
the viscosity of the sol, the ratio of the powder to the sol to be 200 pC N−1 and 4730, respectively (Figure 11f ).
and the sintering conditions.[97] When the ratio of sol to In short, extrusion free forming technology is a relatively
powder was 1:7, green fibers with diameters of ≈300 mm and common technology that has a range of potential applications
lengths of greater than 10 m can be extruded (Figure 11e). in industrial scale production. Moreover, the process has the
Figure 11b demonstrated the microscopic high-density advantages of low production costs, high mechanical stability,
structure of the sintered fiber at 1200 °C. A fiber composite no material size limitation, high material utilization rate, high
material with 1–3 connectivity was fabricated and tested for flexibility, and no need for self-supporting materials. However,
performance. The ferroelectric and piezoelectric properties this process is only applicable to the piezoelectric devices with
were smaller than that of bulk materials (Figure 11g,h).[98] a simple structure. The production of the devices has the disad-
The saturation polarizability and residual polarizability vantages of the poor precision and accuracy, the low resolution,
of the fiber composite material are also not as high as that and the weak piezoelectric performance. Therefore, it is more
of the bulk sample. Kim et al. used a slurry extrusion pro- suitable for the production of bulk devices with low precision
cess to produce BT bulk ceramics (Figure 11d). Figure 11c requirements.
Figure 12. a) Schematic diagram of the projection μSL system for ceramic components. Reproduced with permission.[85] Copyright 2019, Elsevier B.V.
b) Illustration showing the piezoelectric polymer composite materials with BT nanoparticles (orange circles) grafted to a PEGDA matrix (black lines).
Reproduced with permission.[86] Copyright 2014, American Chemical Society. c) Schematic illustration of the surface functionalization method and
strong bonds between the nanoparticles and the polymer matrix after the UV curing process. Reproduced with permission.[74] Copyright 2019, Springer
Nature. d) Schematics of green-part fabrication and postprocesses. Reproduced with permission.[87] Copyright 2016, Elsevier B.V. e) SEM images of
3D-printed piezoelectric microlattices. Reproduced with permission.[74] Copyright 2019, Springer Nature. f) Optical microscopy images of 3D-SAA with
a 64 pillars annular segment array and the concaved-shaped piezoelectric element (PF-CPE). Reproduced with permission.[87] Copyright 2016, Elsevier
B.V. g) Variation of permittivity with temperature for the printed KNN samples.[85] h) Ferroelectric hysteresis (P–E) loops of the printed KNN samples.
Reproduced with permission.[85] Copyright 2019, Elsevier B.V. i) Plot showing the effective piezoelectric modulus (d33) of a grafted PEGDA/BT com-
posite material as a function of BT mass loading.[86] j) Voltage response of various unpoled and poled composite materials (neat films) cycled with a
1.44 N load applied perpendicular to the surface of the film. Reproduced with permission.[86] Copyright 2014, American Chemical Society. k) Schematic
of the test system setup for pulse-echo detecting and ultrasonic imaging. Reproduced with permission.[116] Copyright 2019, MDPI journals. l) Pulse-echo
waveform and frequency spectrum of the transducer array. Reproduced with permission.[91] Copyright 2018, Elsevier B.V.
2.3. Plane to 3D Part-Based Method displacement, but also can improve the flexibility of the fabri-
cated devices.
2.3.1. Stereolithography-Based Printing Moreover, the digital optical masks proposed in recent years
have shown good piezoelectric performance and application
Microstereolithography (μSL) is a new type of microfabrication prospects. Kim et al. chemically modified BT nanoparticles
technology developed on the basis of the traditional additive with acrylate surface groups (Figure 12b),[86] and incorporated
manufacturing process and stereolithography. Compared with them into a solution of easy photo polymerization such as
traditional SLA process, it uses a smaller laser light spot, the polyethylene glycol diacrylate (PEGDA), and exposed them
resin undergoes the photocuring reaction in a very small area, to dynamic changes to generate a digital optical mask with
and the layer thickness is usually 1–10 µm. It has the charac- a defined 3D microstructure, thus enabling fabrication of a
teristics for simple operation, high resolution, and high preci- piezoelectric polymer. The experimental results indicate that
sion of manufacturing devices.[79,85] Based potassium niobate when the mass fraction of the chemically modified BT nano-
(K0.46Na0.5Li0.04Nb0.95Sb0.05O3, KNN) based lead-free piezoelectric particles is 10%, the d33 value of the composite material reaches
ceramics have been fabricated (Figure 12a) by μSL.[85] Using the 40 pC N−1 (Figure 12j). The voltage response of various elec-
dielectric constant and dielectric loss of KNN ceramics printed trodeless and polarized composite materials (pure films) recy-
at different frequencies, it was determined that the maximum cled under a load of 1.44 N perpendicular to the film surface
dielectric constant appeared at 230 °C (Figure 12g). Under increased its output voltage (Figure 12i), which improved the
an electric field of 40 kV cm−1, the spontaneous polarization, mechanical stress transfer efficiency of piezoelectric nano-
residual polarization, and coercive field were Ps = 22.7 µC cm−2, particles. The method not only provides technical support for
Pr = 12.1 µC cm−2, Ec = 6.1 kV cm−1 (Figure 12h), d33 value fabricating 3D piezoelectric polymers, but also lays the founda-
can reach 170 pC N−1. The performance of KNN piezoelectric tion for making high-efficiency piezoelectric polymer materials
ceramics is similar to that of 2D piezoelectric array fabricated through nanointerface tuning.
by traditional cutting methods. These results suggest that μSL Mask image projection stereolithography (MIP-SL), as a
can be used as an alternative method for manufacturing KNN- new type of stereolithography, has also been used to make the
based lead-free piezoelectric ceramic components, especially in high-resolution piezoelectric devices. This experiment used
the production of ceramic devices with complex structures. 70 wt% BT slurry to fabricate cylinders with a diameter of
The μSL technology is used not only in the fabrication of 10 mm and different thicknesses through MIP-SL method.[116]
the KNN ceramics, but also in a 3D piezoelectric PZT ultra- The piezoelectric constants of different cylinders were meas-
sonic array.[91] The PZT array has a d33 of 345 pC/N and a dielec- ured. The d33 value ranged from 146 to 160 pC N−1, and the
tric constant of 1040. On the basis of the array, a 2D ultrasonic dielectric constant and dielectric loss ranged from 1300 to
transducer array (8 × 8) was designed and manufactured with a 13 500 and from 0.018 to 0.02, respectively. Figure 12k revealed
center frequency of 2.24 MHz, and its performance is compa- the performance of the annualar array transducer. The central
rable with that of a traditional 2D piezoelectric array (Figure 12l). frequency of the piezoelectric array is 6 MHz, and its stability
With the continuous development of μSL, Cui et al. made was good. Chen et al. produced a 3D-SAA with 64 cylindrical
piezoelectric materials with arbitrary piezoelectric coefficient arrays and a concave piezoelectric element using a high solids
tensors through design and manufacturing routes.[74] Based content BT slurry with MIP-SL (Figure 12f).[87] Figure 12d
on the electronic displacement diagram of the structural ele- indicated the density change before and after sintering. After
ment pattern family, a perovskite piezoelectric nanocomposite sintering, the density was 5.64 g cm−3, which is a significant
lattice with a complex 3D structure was fabricated by additive increase. The piezoelectric constant and relative dielectric con-
manufacturing. The voltage response of the activated piezo- stant of ceramics produced by the MIP-SL process were 160 pC N−1
electric metamaterial in a given mode is selectively suppressed, and 1350, respectively. The hysteresis loop of the sintered
reversed or enhanced by the applied stress. In addition, using sample revealed good symmetry. This process can be applied
a part of the base material can achieve a higher specific piezo- to biomedical imaging, energy harvesting, and high-intensity
electric constant and controllable flexibility. The team first focused ultrasound. After further research, it was found that
functionalized PZT particles with surface linker loadings of with an increase in BT mass fraction, the grain size increased
0% to 150% (Figure 12c). Then, particles with different degrees significantly and the pore size decreased. When reaching
of functionalization were mixed with an ultraviolet light cured 80 wt% BT, the density was relatively high.[87] A ceramic disc
(UV-cured) resin with volume loading rates of 3% to 30%, and with a diameter of ≈10 mm and a thickness of ≈0.6 mm was
the piezoelectric microlattice of Figure 12e was produced. The fabricated, and its d33 value was measured to be 166 pC N−1.
experiment found that for the composites with low particle The printed samples showed temperature-dependent dielec-
loadings, the unfunctionalized d constant is almost zero, and tric constant and dielectric loss at 1 kHz. All printed samples
it increases with increasing functionalization level. Composite showed only a dielectric peak at ≈120 °C, which corresponds to
materials with high particle loading (30 vol%, 76.3 wt%) also the curing temperature. The 1.4 MHz focused ultrasound array
showed the same trend. With the fully functionalized nanopar- fabricated with this slurry has a −6 dB bandwidth of 40% and
ticles, d increased from 50 to 100 pC N−1. The covalent bond insertion loss of 50 dB at the center frequency. Although this
between the concentrated piezoelectric nanocrystals and the process has many advantages, the performance of its piezo-
embedded UV-sensitive monomer can produce a high-voltage electric device is still far below that from the traditional process.
electric coefficient under a given volume load. This design To sum up, SLA technology is based on the use of UV-
not only can realize the free manipulation of the electrical cured materials and the construction of 3D structures in the
Figure 13. a) SEM images of CNT-coated PA11/BT composite powders. b) Size and size distributions of the CNT-coated PA11/BT composite powders.
c) Schematic illustration of the location of BT and CNT nanoparticles in the SLS-printed PBCNCs-3D composite parts. (Note: the black lines, white
balls, and yellow regions represent CNTs, BT nanoparticles, and the interfaces formed by the sintering of adjacent particles, respectively. The red round
dashed regions represent the microcapacitors in the composite.) d) Frequency dependence of dielectric constant of SLS-printed BT60, PBCNCs, and
PBCNCs-3D parts at room temperature. e) Piezoelectric strain coefficient d33 of the BT60, PBCNCs, and PBCNCs-3D. f) P–E hysteresis loops of BT60,
PBCNCs, and PBCNCs-3D at 100 Hz at room temperature. Reproduced with permission.[117] Copyright 2018, Elsevier B.V.
polymerization process by UV, which has the characteristics 1 kHz, the dielectric constant of the PBCNCs-3D component
of high resolution and high surface finish. The manufactured was 16.2, which is approximately twice that of the SLS-produced
piezoelectric ceramic device has the advantages of high electro- composite component (PBCNC) without the isolation structure
mechanical conversion efficiency and adjustable flexibility. It (Figure 13d). The d33 value increased from 1.7 to 2.1 pC N−1
can be extended to other functional materials to achieve high- (Figure 13e). Figure 13f revealed that the degree of polarization
fidelity printing of complex 3D functional structures. Although increased with the construction of the 3D isolation structure in
there are many advantages to adopting this process, the piezo- the PBCNCs-3D sample. This not only provides new materials
electric devices fabricated have poor stability, low responsive- for the fabrication of piezoelectric devices by the selective laser
ness, and printing speed, and the process equipment still needs melting (SLM), but also establishes a foundation for improving
to be improved. the performance of piezoelectric polymer composites by con-
structing a 3D separation flow path.
In addition, the magnetoelectric material is also a kind of
2.3.2. Selective Laser Sintering material with piezoelectric effect, and a new material combina-
tion method was proposed to realize 4D printing by producing
SLS technology utilizes a moving laser beam to track and selec- piezoelectric effect. A functionality of the integrated device
tively sinter powdered polymers or metal composites into a con- fabricated by 4D printing is endowed to transfer mechanical
tinuous cross-section of 3D parts. No self-supporting structure to electrical energy based on the electromagnetic introduc-
is needed, the production cost is low, and it is suitable for the tion principle.[31] The porous structure was firstly fabricated
fabrication of larger devices.[79,117] Qi et al. prepared polyamide 11 using the composite powders by the SLS process. Then, the
(PA11)/BT/carbon nanotube (CNT) ternary nanocomposites conductive helix structure constructed from the porous struc-
(PBCNCs-3D) by the SLS.[117] SEM images of conventional ture magnetized and connected with two flat plates was fab-
composite powder and the PA11/BT composite powder coated ricated by the SLM process. When the integrated 4D printed
with CNTs are shown in Figure 13a. The particles of both pow- devices were compressed by 40%, the output voltage attained
ders presented irregular shapes and rough surfaces. Figure 13b 11.8 µV. Such 4D printing process may lay the foundation for
demonstrated that the average particle size of PA11/BT com- performance-changed and functionality-changed 4D printing by
posite powder coated with traditional composite powder and putting forward a material combination concept.
carbon nanotubes were 50 and 42 µm, respectively, and the par- The SLS process has the advantages of good surface finish,
ticle size distribution of the powder is basically in the optimal high mechanical stability, and easy control of device structure
range for the SLS process. The 3D segregated conductive and size. However, because of its high laser intensity, its low
pathway was efficiently constructed in the PBCNCs-3D parts versatility is mostly useful for metal materials. In addition, the
with a low percolation threshold of 0.3 wt% (Figure 13c). At SLS process has the disadvantage of slow printing speed. Owing
to the precision of devices depending on the size of powder x-100 dispersant, ethanol, diphenyl (2,4,6-trimethylbenzoyl) phos-
particles, and there are high requirements with respect to the phine oxide, and acrylamide monomer to obtain a KNN slurry
slurry. Moreover, the raw material is powder with the larger size that could be used in microstereolithography method.[85] A 2D
generally, so the surface of the printing device is rough. These segmented ultrasonic array was fabricated with the slurry to test
reasons limited the development of SLS process. the phase structure of the material surface. Figure 14c demon-
strated the changes degreasing and sintering. For example, after
debonding, the material surface showed a large porosity, while
3. Additive Manufacturing of Piezoelectric after sintering, the surface density was significantly increased.
XRD revealed that the crystallization performance of the sample
Materials
was good (Figure 14f). Furthermore, the lead-based ceramic
The production of printable ink is the main step in additive powder as the slurry was also investigated. The PZT slurry with a
manufacturing, which directly affects the performance of best ratio of PZT:resin = 87:13 was prepared, and a high viscosity
piezoelectric devices. Typical printable ink components include of 3100 cPS can be achieved.[91] With increasing PZT content,
fillers, dispersants, solvents, and adhesives. The choice of the grain size increased and the surface density was enhanced
these components depends largely on the printing method. (Figure 14b). XRD showed that all samples have a perovskite
Fillers are the active ingredients of inks and provide the spe- crystal structure (Figure 14e). The crystallinity saturation reached
cific functions required. Fillers can be metals, organics, poly- to greater than 87%. In addition, Cha et al. mixed BT powders
mers, or combinations, depending on the application. With the of different weight percentage with a photosensitive resin by
rapid development of nanotechnology, researchers have been ball milling.[122] Adding dispersant to improve the dispersion
able to synthesize specific nanomaterial inks. The achieve- of the slurry, a photocurable slurry can be obtained. SEM sug-
ments in additive manufacturing technology in nanomaterials gested that the density increased with increasing BT percentage
have brought about tremendous developments in the progress (Figure 14a). The crystallization performance also improved grad-
of the electronics field. Another important component of ink ually (Figure 14d), reaching the saturation state at 87%.
is the solvent. Solvent is an important medium for ink flow, For additive manufacturing of piezoelectric ceramics, com-
and it should have good solubility. The choice of solvent is par- pared with the traditional process, the functional characteristics
ticularly important in the printing of multilayer equipment. are similar, and additive manufacturing technology can be used
When new ink is printed on the printing film, the solvent of for the structure of complex, high precision micro and small
the ink may dissolve and damage the underlying printing film. devices, which are more suitable for the production of piezo-
This problem can be solved by adjusting the solvent compo- electric ceramic devices. There is a need to continue to explore
sition of the ink. In addition to these, additives such as dis- the slurry preparation as the main part of the additive manufac-
persants and surfactants that change the rheology, wettability, turing. At present, the enhancement of the material performance
or tensile properties of the ink are needed. By adjusting the primarily occurs by doping to promote the physical and chemical
proportion of each additive, an ink with better rheology, vis- properties of the material. In this case, the piezoelectric, the sen-
cosity, and dispersibility can be prepared. Ink is the basis of sitive conductivity, the chemical sensitivity, and the mechanical
additive manufacturing of devices, and the composition is strength of the materials can improve. While preparing ceramic
complex. Therefore, the investigation of the composition for slurry, the mixing mode, proportion, and size of ceramic powder
the printing ink is an indispensable part of additive manu- should be fully considered. If the ceramic slurry is not prepared
facturing. General slurries are inorganic ceramic materials, properly, it may lead to deposition and suspension of the ceramic
organic polymer materials, and composite materials, which are slurry, which may affect the performance of the printing devices.
introduced in turn. In addition, piezoelectric ceramic materials that can be applied
in additive manufacturing still need to be developed.
3.1. Rigid Piezoelectric Ceramics

3.2. Piezoelectric Polymer Materials
As an electronic ceramic material with excellent piezoelectric
properties, piezoelectric ceramics have unique ink-forming PVDF is a semicrystalline polymer with repetitive units (CH2–CF2)
capacity and viscoelasticity. After annealing treatment, the piezo- that has high fracture strength, good thermal stability, easy
electric ceramic material can be placed under a strong electric processing, good biocompatibility, and other inherent excellent
field for polarization after the electrode is added to the end face. characteristics. PVDF can be turned into four different crystalline
After the polarization treatment, the piezoelectric properties of phases: α, β, γ, and δ. The α phase is polar and shows no unique
the ceramics are improved. In addition, piezoelectric ceramic electrical response; the electrical activity of the β phase (trans)
materials also have the advantages of low cost, good piezo- resulting from the dipole moment interacting with a sawtooth
electric performance, easy integration, low energy loss. Based wave shape causes the polarity to increase. Therefore, its high
on these factors, piezoelectric ceramic materials are widely used piezoelectric constant and ferroelectric constant, as well as high
in additive manufacturing. Researchers are increasingly inter- piezoelectric responsiveness, has become the focus of research.
ested in the composition of piezoelectric ceramic slurries.[118–121] In the past few years, the development of additive manufacturing
A KNN slurry was prepared as follows. First, KNN powder PVDF structures has made rapid progress. Because of its excel-
was prepared by a solid phase method. A fine powder was then lent flexibility and ability to enhance the piezoelectric coupling
obtained by ball milling. KNN powder was mixed with triton factor by increasing the extractability of the structure, research on
Figure 14. a) SEM microstructures of the surface with different PZT powder different contents. Reproduced with permission.[122] Copyright 2019, The
Korean Ceramic Society. b) SEM images of printed BT ceramics with different contents. Reproduced with permission.[91] Copyright 2018, Elsevier B.V.
c) SEM images of the debonded KNN green parts and the sintered samples. Reproduced with permission.[85] Copyright 2019, Elsevier B.V. d) XRD pat-
terns of sintered ceramics with different PZT contents. Reproduced with permission.[122] Copyright 2019, The Korean Ceramic Society. e) XRD patterns
of BT ceramics with different weight percentages. Reproduced with permission.[91] Copyright 2018, Elsevier B.V. f) XRD patterns of the KNN calcined
powders and sintered samples printed by μSL technology. Reproduced with permission.[85] Copyright 2019, Elsevier B.V.
the preparation of PVDF slurries has been increasing day by day. significantly and the viscosity also increased (Figure 15di). It
Currently, PVDF structures for additive manufacturing have been can be seen from the SEM images in Figure 14dii–iv that when
used in energy collectors, drivers, and sensors.[123–125] the concentration of PVDF exceeds 35 wt%, the composite vis-
The preparation method for PVDF slurry is usually to dis- cosity of the resin is greater than 200 Pa s. The resin was no
solve PVDF and then to adjust the viscosity of the solution; the longer stable on the manufacturing platform for 30 s, which led
process is simple and easy to operate. In a previous experiment, to an uncontrollable recoating step, thus affecting the dimen-
PVDF powder was mixed with DMF, after which polypropylene sional accuracy of the device. Therefore, 35 wt% PVDF is the
(PR, a clear resin) was added to the PVDF solution, which was maximum concentration in V-ink. The optimized piezoelectric
stirred with a magnetic stirrer. A photoinitiator was added to voltage coefficient (g33) was 105.12 × 10−3 V m N−1.
obtain a PVDF solution that can be used for light curing. The At present, the most commonly used piezoelectric polymer
reaction mechanism is shown in Figure 15a. Bulk precipita- material is PVDF. Therefore, while preparing polymer slurry,
tion polymerization was observed when PVDF and PR were the solvent bonded with PVDF can be selected to form inter-
mixed at a ratio of 1:5 (Figure 15b).[93] The blends of 5 wt% molecular forces, and increase dipole orientation density,
PVDF/PR by additive manufacturing without DMF solution, and improve dipole orientation and mechanical tension, thus
2 wt% PVDF/PR without DMF solution, and 5 wt% PVDF/PR enhancing the piezoelectric performance of the polymer
after DMF solution were analyzed by SEM. The experimental materials. In addition, the amount of solvent and infill propor-
results demonstrated that with an increase in the amount of tion will also affect the device stress, the mechanical force, and
PVDF, the sample surface became rough and the PVDF did so on. The performance of a polymer slurry generally depends
not agglomerate, showing a good matrix structure (Figure 15c). on the solvent and the amount of solvent used. At present, the
Furthermore, additive manufacturing process based on photo- technology regarding the production of piezoelectric polymer
controlled polymerization technology for an all-polymer-based slurry is not fully mature enough.
piezoelectric photocurable resin (named V-ink) was also
studied. The V-ink used PVDF powder (Sigma-Aldrich) as
the piezoelectric material, 1,6-hexanediol diacrylate monomer 3.3. Piezoelectric Composites
(HDDA, Sigma-Aldrich) as the matrix material, and diethyl
fumarate (DEF, Sigma-Aldrich) as the solvent to adjust the vis- Composites are formed by combining at least two materials
cosity of V-ink.[126] As the PVDF concentration changed from according to the desired product characteristics. There are ten
25, and 37.5 to 50 wt%, the piezoelectric coefficient improved possible modes of connection in two-phase mixing, from 0–0 to
Figure 15. a) Schematic representation of the photopolymerization of the methacrylate monomer and oligomers along with the PVDF solution in
DMF.[93] b) Bulk precipitation polymerization observed when PVDF was mixed with PR in a 1:5 ratio.[93] c) SEM images of the surfaces of printing blends.
Reproduced with permission.[93] Copyright 2019, Cambridge University Press. di) Complex viscosity for V-ink with various concentration of PVDF.[126]
(dii–iv) SEM images of printed examples of V-inks with varying concentration of PVDF particles at different contents. Reproduced with permission.[126]
Copyright 2017, Elsevier B.V.
3–3. Some of these connection modes are particularly suitable order to further improve the piezoelectric performance of
for separating longitudinal and transverse piezoelectric effects, composite materials, PVDF and BT NPs were mixed by ball
significantly enhancing the piezoelectric properties of the mate- milling, extrusion, and ultrasound, and the effects on the PVDF
rial. The piezoelectric composite materials have high dielectric β phase were analyzed and compared.[75] For samples made by
constant, low dielectric loss, high energy storage density, and the ultrasonic technique, the α peak is at 18.7°. In the extruded
large breakdown strength. Therefore, the research of composite mixed sample, the α peak is significant at 40°, and the γ peak
materials is also favored by researchers. Piezoelectric compos- is near 26°. However, there are no peaks at 18.70°, 20.04°, and
ites are important for various emerging applications, such as 26.50° for the PVDF α phase in the nanocomposite prepared by
wearable electronic devices, sensors, energy storage devices, ball milling. There exists that single broad peak at 2θ value of
and biomedical devices. Combine this superior material with 20.26° corresponding to the (200) and (110) planes of β phase.
the flexibility of additive manufacturing and you have an even The experimental results suggest that the nanocomposite films
brighter spark.[9,127,128] prepared by ball milling only crystallized in the β phase. The
Kim et al. used a nanocomposite filament by mixing PVDF ball milling had no effect on the performance of BT NPs, and
with BT powder.[107]The surface morphologies of printing its peak position did not change. It can be seen from the SEM
composite films with different BT fillers were compared by images (Figure 16b) that the highly porous structure of the
SEM analysis, as shown in Figure 16a. With an increase in nanocomposite prepared by ball milling caused its mechanical
the content of BT filler, the size and filler aggregates in PVDF modulus to decrease, making it more suitable for the mixing of
matrix were relatively increased, and the porosity in the matrix PVDF and BT NPs.
was also increased. However, when the amount of BT was Piezoelectric composites are a direct way to improve the per-
15 wt%, the cohesion and defects were the largest, and the formance of piezoelectric devices, so researchers are increas-
tensile strength and toughness were reduced. But BT was 15 wt%, ingly enthusiastic about the fabrication of piezoelectric compos-
PVDFs axial and output currents increased significantly. In ites. The choice and proportion of the fillers are the primary
Figure 16. a) SEM images of the surfaces of printing composite films with different compositions. Reproduced with permission.[107] Copyright 2017,
Wiley-VCH. b) SEM images of the surfaces of films fabricated from 0.2 g mL−1 solutions of nanocomposites prepared by (i) ball milling, (ii) extrusion,
and (iii) sonication. (Yellow circles highlight the BaTiO3 NPs agglomerates) (printing parameters: 1 MPa at 20 mm s−1 with a 100 µm nozzle).
Reproduced with permission.[75] Copyright 2017, American Chemical Society.
issues in the preparation of composite slurries, which seriously 1) Electromechanical response: The electromechanical
affect the rheological properties, the shear stress, the mechan- response can be changed directly from the 3D design. This
ical force and the surface tension of the materials. The compat- change is due to the synergistic enhancement of approach-
ibility between the filled materials needs to be considered. In able strain and coupling between the in-plane and out-of-
addition, the way of the slurry is prepared also affects the prop- plane piezoelectric coefficients, increasing the voltage output
erties of the material. The mechanical strength, structural pre- and the sensitivity of the device, and improving the electro-
cision, and piezoelectric properties of composite slurry printing mechanical conversion efficiency. This 3D electronic inte-
devices can be clearly enhanced. gration method effectively increases the electromechanical
responsivity, which plays an important role in improving the
sensing efficiency of piezoelectric sensors, the frequency of
4. Summary focused ultrasonic systems, and the collection efficiency of
energy collectors.[75,86,87]
With the rapid development of the human society, the exploring 2) Piezoelectric constant: Piezoelectric materials made by tradi-
and the application of functional materials have become the tional methods have a charge motion that is regulated by the
focus of researchers’s attention. Improving the piezoelectric internal crystal, and the crystal orientation is relatively disor-
sensor efficiency, enhancing the precision of the device, and dered, which inhibits the material performance. The additive
increasing the electromechanical response to improve the manufacturing method can manipulate and design arbitrary
performance of the piezoelectric device so that the piezo- piezoelectric constants, allowing users to specify and pro-
electric material can be more widely used have become hot gram voltage responses through 3D active topologies, ena-
discussion topics. In the traditional sense, improving the per- bling free combinations of arbitrary piezoelectric constants
formance of piezoelectric devices usually is accomplished by in the material and amplifying, reversing or suppressing
improving the material itself, such as doping, coating, and them in any direction. If applied to the piezoelectric sensors,
other methods. The emergence of additive manufacturing it can not only enhance the flexibility and responsiveness of
technology provides a new method for the fabrication of the sensor, but also accurately judge the position, size, and
piezoelectric devices and the improvement of the performance direction of the impact at any position by responding to the
of piezoelectric devices (Figure 17). It changes the device mechanical pressure, impact force, and vibration through
production process to improve the performance of the device. the electrical signal.[74]
The application of additive manufacturing technology to the 3) Material properties: By adding a certain proportion of
fabrication of piezoelectric materials is becoming a popular organic material and further modifying the material, the flex-
trend in device fabrication. ibility of the material can be effectively increased. Adjusting
Figure 17. Advantages of additive manufacturing of piezoelectric materials. Reproduced with permission.[74] Copyright 2019, Springer Nature. Repro-
duced with permission.[75] Copyright 2017, American Chemical Society. Reproduced with permission.[105] Copyright 2018, Elsevier B.V. Reproduced with
permission.[129] Copyright 2015, American Chemical Society.
the rigidity and shape of a material can help the material to improve the piezoelectric devices. It is necessary to design
achieve tunability and versatility, enabling it to be formed a multiphase system, through accurate and reasonable con-
into thin slices or hard blocks similar to gauze strips. Piezo- trol of the proportion of components, without them affecting
electric elements made of this additive are adjustable and each other, so that the inherent advantages of components
versatile, and can self-inductively synthesize skin to record can be utilized, and various materials to enhance the perfor-
and detect pressure. They can also be used as energy har- mance of piezoelectric composites can be discovered, to pro-
vesting devices, wrapping them around arbitrary curvature to mote the development of additive manufacturing of piezo-
make the device thick, light, hard, or able to absorb energy.[74] electric devices.[130–133]
4) Size shape: To control the size and shape of the device, tradi-
tional methods such as etching and cutting technology have
been used, which generate mechanical stress that can lead 5. Prospects
to grain loss, strength degradation, and near-surface-area
depolarization, resulting in a significant reduction in the In this paper, several advanced additive manufacturing tech-
performance of the piezoelectric element. Forming a piezo- nologies and the latest progress in piezoelectric materials are
electric array with a complex shape using these methods described. Although additive manufacturing technology has
is challenging, and brittle ceramics cannot be shaped into made great achievements in the fabrication of piezoelectric
a higher order 3D structure. The additive manufacturing devices, there are still some problems that need to be solved
technology with high resolution can realize the fabrication before it can be applied in a wider field and commercialized
of complex shapes and precise structures, eliminating the (Figure 18).
extra manufacturing steps. It can not only improve the preci-
sion of piezoelectric devices, but also effectively enhance the 1) Improvement of the compatibility between raw materials and
performance of piezoelectric devices, such as the mechanical printing technology: Ink generally contains other additives to
response, sensitivity, and sensing efficiency. It can be used as adjust the thixotropy and rheological property of piezoelectric
a long-term solution for the fabrication of fine devices and materials. For piezoelectric composites, the interaction
complex devices. The additive manufacturing of piezoelectric strength between the interface, the compatibility between
devices will further promote the development of piezoelectric raw materials and additives, and the slurry and printing pro-
materials for wider applications.[87] cess must be carefully considered, as these may affect the
5) Multiphase doping: Regarding multiphase doping research physical properties, chemical properties, and mechanical
of piezoelectric materials, the graphene, carbon nanotubes, strength of the piezoelectric materials. Therefore, it is urgent
nanofiber, and the performance of materials such as poly- to develop additives suitable for piezoelectric materials, and
ethylene glycol acrylate doped into the piezoelectric material further exploration is needed. In addition, the ratio between
system have been studied enhance the dielectric constant and the material proportion and additives should be studied. The
piezoelectric constant of piezoelectric devices to improve the different proportions will affect the piezoelectric properties,
mechanical and electrical response of piezoelectric devices and dielectric properties, electromechanical coupling con-
and piezoelectric sensitivity. Multiphase doping is a trend of stants of materials, so we should spend time and energy to
additive manufacturing slurry preparation. As the number study the proportion problem to make ink with better perfor-
of components in the system increases, the mechanism mance in all aspects, which can facilitate the mass produc-
increases in complexity, and there are more opportunities to tion of piezoelectric devices in the future.
piezoelectric performance and sensitivity as the density and

precision of piezoelectric devices are further improved. With
the development of technology, new materials need to be
explored and developed continuously. Only when the two pro-
ceed in parallel can the performance of piezoelectric devices
improve and the number of applies fields increase. At pre-
sent, three major components related to improving the prop-
erties of raw materials, namely, domain engineering,[135,136]
orientation engineering,[137,138] and strain engineering,[139–141]
have been proposed to improve the piezoelectric properties
of materials by changing the structure size of the domain,
adjusting the orientation of the crystal structure, and regu-
lating the growth and morphology of nanoparticles. Strain
engineering, as an important physical parameter in additive
manufacturing of piezoelectric materials, plays a crucial role
in the fabrication of piezoelectric devices. The heterogeneous
epitaxial interface of piezoelectric materials can be con-
structed by additive manufacturing technology and interface
strain engineering to improve the piezoelectric performance.
In the construction of a heterogeneous epitaxial interface,
the substrate phase is used as a template or substrate. Along
a crystal phase of the substrate phase, the heterogeneous epi-
taxial orientation is used to grow another texture phase with
Figure 18. Prospects for future development to piezoelectric materials
prepared by additive manufacturing.
little difference from the lattice constant of the substrate.[142]
The coexisting crystal phase with little difference in crystal
structure is constructed and the heteroepitaxial interface
2) Improvement of postprocessing process: Additive manufac- is formed. By regulating the binding state at the interface,
turing of piezoelectric devices whose size and structure are such as lattice matching, interface composition, stress and
on the sub-micrometer or even nanoscale can be achieved, strain,[143] residual polarization is improved,[144] polariza-
where each layer of the structure present an orderly tion rotation is promoted,[145] and spontaneous polarization
arrangement, revealing excellent precision and density. The and domain wall motion speed are enhanced. Therefore,
alignment of sub-micrometer and nanoscale structures is the implementation of interface strain engineering is also a
important for the sensitivity and piezoelectric properties comprehensive application of orientation engineering, elec-
of piezoelectric devices. Like devices made by traditional tric domain engineering, and morphotropic phase boundary
methods, additive manufacturing of piezoelectric devices construction. As long as the above methods all show good
usually requires high temperature treatment, which is a time synergy, appropriate regulation of heteroepitaxial interface
consuming and complicated process. After degreasing and density, exploration of the heteroepitaxy interface density[146]
sintering, the photosensitive resin and other additives vola- and correlated piezoelectric properties, combined with addi-
tilize, exposing the micropores and reducing the sensitivity, tive manufacturing technology, can effectively improve the
sensing efficiency and responsivity of piezoelectric devices. performance of the piezoelectric devices. Therefore, using
It is difficult to produce these devices on a large scale, interface strain engineering for high performance research
requiring the development of more advanced or higher den- of piezoelectric materials is promising. Our previous study
sity and finer surface resolution finer without the need for found that piezoelectric properties can be effectively regu-
postprocessing technology. This is an issue that the future to lated by adjusting the heteroepitaxial interface density
additive manufacturing technology must address to continue and lattice mismatch rate of the titanate nanocomplex. By
its development.[134] adjusting the proportion of two-phase components in the
3) Development of active piezoelectric materials: There are a binary titanate nanocomplex, the piezoelectric properties
limited amount of materials that can be printed, especially can be regulated. It is preliminarily found that when the
active materials whose physical properties, surface topolog- proportion of two-phase components is close to 1, it can be
ical structure, and geometric dimensions can be engineered regarded as the maximum density of the heterogeneous
and intelligently produced. As a prerequisite for application epitaxial interface, and the piezoelectric properties are the
in additive manufacturing technology, ink should have the highest.[147,148] Proper adjustment of the lattice mismatch rate
appropriate surface tension, surface activity, and rheological of different binary titanate nanocomplexes could also effec-
properties. However, most piezoelectric active materials are tively regulate the piezoelectric properties.[149–151] This is due
inorganic materials, so it is imperative to explore new active to the adjustment of the binding state at the interface, such
piezoelectric materials to improve the piezoelectric perfor- as lattice matching, interface components, stress and strain,
mance of devices. to improve residual polarization, promote polarization rota-
4) Exploration of new materials and systems: Additive manufac- tion, and enhance the spontaneous polarization ability and
turing technologies continue to evolve, resulting in increased domain wall motion speed.[152–154] In addition, the oriented
polycrystal not only suggests the excellent piezoelectric human blood pressure, electrocardiograms, and heat consump-
performance of a single crystal, but also reflects the perfor- tion. The wireless network can transmit information to the
mance superposition multiplier effect brought about by the Internet and the IoT in real time and provide reasonable health
uniform orientation of the polycrystalline structure.[155,156] advice through cloud computing. With the continuous develop-
The construction of high-density heteroepitaxial interface- ment of printing technology and piezoelectric materials, addi-
oriented piezoelectric nanocomplex provides a path for the tive piezoelectric devices with long-term durability, good safety,
development of new high-performance lead-free piezo- and high energy, high density, and high power are expected to
electric materials and has great potential for the fabrication be used in a wider range of fields.
of high-performance piezoelectric devices.
5) Improvement of packaging technology: The packaging of
piezoelectric components plays a role in the mechanical Acknowledgements
and environmental protection of the circuit, so that it can
improve the stability, safety, and service life of electronic This work was supported in part by the National Natural Science
components. However, the packaging of electronic compo- Foundation of China (No. 21005003), the Natural Science Basic
Research Plan in Shaanxi Province of China (2019JM-091), the Serving
nents made of piezoelectric materials is still difficult, and the Local Scientific Research Project in Foundation of Shaanxi
the lack of rigorous top design in the industrialization of Education Department of China (19JC002), and the Doctoral Scientific
piezoelectric materials limits the application of piezoelectric Research Starting Foundation of Baoji University of Arts and Sciences
materials. Effective packaging in additive manufacturing (No. ZK2018059).
of piezoelectric devices is also critical for the protection of
devices from physical and chemical damage. Therefore,
new technologies and materials for printing and pack- Conflict of Interest
aging piezoelectric elements are also worthy of further
research.[157,158] The authors declare no conflict of interest.
6) Adding smart materials for complex device fabrication: On
the basis of existing piezoelectric raw materials, smart struc-
tural materials that can automatically recover their initial Keywords
shape under external stimulation, such as electricity, light,
additive manufacturing, oriented nanomaterials, piezoelectric devices,
magnetism, heat, or solution, can be employed to realize 4D piezoelectric materials, slurry preparation
printing of piezoelectric devices. Adding materials to shape
memory can be used to make soft circuits and shape memory Received: June 17, 2020
objects with response circuits. Such response objects can Revised: August 15, 2020
be used to make soft robots, sensors for minimally invasive Published online:
medical devices and wearable electronic devices, so they have
a broad application prospects. Moreover, additive manufac-
turing can overcome the poor processing characteristics of
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Cheng Chen is currently a postgraduate student in Faculty of Chemistry and Chemical

Engineering, Engineering Research Center of Advanced Ferroelectric Functional Materials, Baoji
University of Arts and Sciences, China. She received B.S. degree from Baoji University of Arts and
Sciences (2019). Her current research is focused on development and application of BaTiO3-based
piezoelectric nanocomposites.
Xi Wang is currently a postgraduate student in Faculty of Chemistry and Chemical Engineering,

Engineering Research Center of Advanced Ferroelectric Functional Materials, Baoji University of
Arts and Sciences, China. She received B.E. degree from Baoji University of Arts and Sciences
(2019). Her current research is focused on the development of piezoelectric composites and
energy capture device.
Yan Wang is currently a postgraduate student in Faculty of Chemistry and Chemical Engineering,
Engineering Research Center of Advanced Ferroelectric Functional Materials, Baoji University of
Arts and Sciences, China. She received B.S. degree from Baoji University of Arts and Sciences
(2018). Her current research is focused on BaTiO3 base flexible composite energy storage films
and high-performance piezoelectric nanogenerators for energy harvesting.
Dangdan Yang is currently a postgraduate student in Faculty of Chemistry and Chemical

Engineering, in Engineering Research Center of Advanced Ferroelectric Functional Materials, Baoji
University of Arts and Sciences, China. She received B.S. degree from Baoji University of Arts and
Sciences (2018). Her current research interests mainly focus on the development of perovskite
mesocrystalline piezoelectric nanocomposites.
Fangyi Yao is currently a doctoral student in Faculty of Engineering and Design, Kagawa University,
Japan. She received M.S. degree from Baoji University of Arts and Sciences (2018). Her current
research is mainly focused on the synthesis of inorganic functional materials and fabrication of
high performance reverse osmosis porous membrane for brackish water desalination.
Wenxiong Zhang is currently a postdoctoral researcher at Institute for Solid State Physics, The
University of Tokyo, Japan. In 2019, he received his Ph.D. degree in materials engineering from
Kagawa University, Japan. His current research focuses on development and application of all-
solid-state Li-ion batteries.
Bo Wang is currently an Associate Professor in the School of Materials Science and Engineering,
Xi’an Jiaotong University. He received the B.S., M.S., and Ph.D. degrees from Xi’an Jiaotong
University, Xi’an, China, in 2002, 2005, and 2009, respectively. His current research interests
include materials design for porous ceramics, nanomaterials, and ceramic/polymer composites.
Galhenage Asha Sewvandi obtained her BSc in Materials Engineering and MEng in Manufacturing
Systems Engineering from University of Moratuwa, Sri Lanka. She received her Ph.D. in 2015 at
Kagawa University, Japan. She currently holds a position as a senior lecturer at the Department
of Materials Science and Engineering, University of Moratuwa, Sri Lanka. Her research interests
focus on the simulation, fabrication, and characterization of photovoltaic and dielectric materials.
Desuo Yang is currently a Professor in Faculty of Chemistry and Chemical Engineering, Baoji
University of Arts and Sciences, China. He received B.S. degree from Northwest University (1984),
M.S. degree from Xian Modern Chemistry Research Institute (1987), and Ph.D. degree from
Lanzhou University (2004). His research mainly focuses on preparation and application of fluores-
cent molecular probe.
Dengwei Hu is currently a Professor in Faculty of Chemistry and Chemical Engineering, a director

in Engineering Research Center of Advanced Ferroelectric Functional Materials, Baoji University
of Arts and Sciences, China. He received B.S. degree from Baoji University of Arts and Sciences
(2003), M.S. degree from Northwest Normal University (2009), and Ph.D. degree from Kagawa
University, Japan (2014). During the period from November 2014 to March 2015, he was working
in the Department of Advanced Materials Science, Faculty of Engineering, Kagawa University, as
a postdoctor. His current research is focused on textured nanocomposite piezoelectric ceramics,
flexible piezoelectric devices.

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Additive Manufacturing of Piezoelectric Materials

efficiency and reduced the size of equip-

C. Chen, X. Wang, Y. Wang, D. Yang, Prof. D. Yang, Prof. D. Hu Dr. W. Zhang

We focus on SLA, SLS, solvent evaporation-assisted 3D printing

Table 2. Comparison of additive manufacturing techniques for piezoelectric devices[65,79,109].

Process AM method Available materials Advantage Limitation Applications

3.1. Rigid Piezoelectric Ceramics

piezoelectric performance and sensitivity as the density and

Cheng Chen is currently a postgraduate student in Faculty of Chemistry and Chemical

Xi Wang is currently a postgraduate student in Faculty of Chemistry and Chemical Engineering,

Dangdan Yang is currently a postgraduate student in Faculty of Chemistry and Chemical

Dengwei Hu is currently a Professor in Faculty of Chemistry and Chemical Engineering, a director

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