Resources Chemicals and Materials 2 (2023) 128–142

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Resources Chemicals and Materials

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Review of the applications of 3D printing technology in the field of

piezoelectric ceramics
Dawei Sun a, Yao Lu a,∗, Tomoaki Karaki b
a
Shenyang University of Chemical Technology, Shenyang 110142, China
b
Toyama Prefectural University, Imizi 939-0398, Japan

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

Keywords: As advanced functional materials, piezoelectric ceramics are widely used in various fields, including the medical,
Piezoelectric ceramics aviation, and military industries. With the advancement of science and technology, the piezoelectric ceramics
3D printing technology needed in special fields have become more intelligent, diverse and lightweight. The shapes and structures of
Additive manufacturing
piezoelectric ceramics are becoming more complex. Traditional piezoelectric ceramic preparation technology
has been unable to meet the high-speed and complex production demands of various industries. Considering
this situation, 3D printing technology has attracted much attention in the field of piezoelectric ceramics. In
this paper, the applications of several main 3D printing techniques in the field of piezoelectric ceramics are
mainly introduced, and their development statuses, process characteristics and achievements are summarized.
The advantages and disadvantages of each printing technique are summarized and compared. The challenges and
possible future trends of 3D printing when manufacturing piezoelectric ceramics are summarized and proposed.

1. Introduction
Piezoelectric ceramics are important functional materials that can re-
alize the conversion of mechanical energy to electrical energy and vice
versa. They have the same characteristics as ceramic materials, such as
high strength, hardness, and corrosion resistance values. As functional
devices, piezoelectric ceramics are widely used in ultrasound [1–3],
transduction [4–6], and other equipment, and are widely used in the
medical [7,8], communications [9,10], military science and technology
industries [11,12]. With the development of science and technology,
the update of high-end equipment, in which functional devices have
improved performance levels, high precision development, and piezo-
electric ceramics as functional devices, the shapes and structures of their
compositional requirements are increasingly strict. Although each tra-
ditional molding method for piezoelectric ceramics has its own advan-
tages, the traditional molding methods are often limited when faced
with different molding requirements [13].
The traditional piezoelectric ceramic molding processes mainly in-
clude dry pressing [14], injection molding [15], and cast molding [16].
Dry pressing is a common molding method for molding piezoelectric ce-
ramics. This process has the advantages of easy operation, short process
cycle time, high molding density, low shrinkage, and high mechanical
strength. However, dry press molding is mostly used for small and sim-
ple blanks, such as discs, sheets or rings, which require complicated
processing after molding, and the blanks are prone to cracking and de-
lamination when the pressure in the mold is not uniform [17]. Injection
molding has the advantages of short process cycle time, dense and uni-
form molding, and flexible operation. However, because its injection
process requires colloid as a medium and must be degreased, it eas-
ily leads to high organic content in the blanks, large porosity and easy
cracking after firing. Tape cast molding is mostly used to prepare chip
multilayer ceramic capacitors that exhibit piezoelectric effects [18,19],
the cast process weaves and prepares piezoelectric ceramics with ex-
cellent performance levels, but the process cycle is long and compli-
cated, which lacks practicality during production. In addition, most of
these molding methods require molds and secondary processing of the
samples after forming [20]. Conventional processing methods include
grinding, tool cutting and laser etching, which lead to long processing
periods and the occurrence of undesirable results when processing com-
plex samples.
The traditional molding process for piezoelectric ceramics often fails
to meet the characteristics of a fast molding speed and high molding ac-
curacy, and it is susceptible to the influence of the mold. Due to the
limitations of the traditional processes for preparing ceramics, 3D print-
ing technology with advantages including fast molding, high precision,
three-dimensional modeling, materials technology, digital information
technology, and no physical molds, can achieve the rapid printing of
complex devices [21,22]. For additive manufacturing, 3D printing tech-

∗
Corresponding author.
E-mail address: luyao915@syuct.edu.cn (Y. Lu).

https://doi.org/10.1016/j.recm.2023.02.001
Received 9 November 2022; Received in revised form 15 February 2023; Accepted 18 February 2023
Available online 26 February 2023
2772-4433/© 2023 The Authors. Published by Elsevier B.V. on behalf of Shenyang University of Chemical Technology. This is an open access article under the CC
BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/)
D. Sun, Y. Lu and T. Karaki Resources Chemicals and Materials 2 (2023) 128–142

Table 2
Comparison of piezoelectric properties of piezoelectric ceramics manufactured
by 3D printing technology and traditional technology.

Materials d33 (pC/N) 𝜀r tan 𝛿 Density (g/cm3 )

3D Printing Technology
PZT [42] 283 765 0.02 7
PMNT[43] 620 – – 7.95
PLZT[44] 481 1986 – 7.74
BT[45] 163 2762 0.016 5.69
KNN[46] 170 2150 0.08 4.09
Traditional Technology
PZT[42] 410 1900 0.014 7.5
PMNT[43] 630 – – 8.03
PLZT[47] 108 3895 0.029 7.571
BT[45] 190 1700 0.1 6.02
KNN[48] 160 420 – 4.46

Fig. 1. Advantages of 3D printing technology in the field of ceramics [29–31].

nology greatly reduces the waste of raw materials during subsequent
processing, as shown in (Fig. 1). To date, the 3D printing technolo-
gies for polymer and metal materials have matured. The 3D printing of
polymers has been applied to the aerospace industry for creating com-
plex lightweight structures [23,24], and this technology has been heav-
ily used in the medical and automotive fields [25–28]. However, 3D
printing technology has not yet been applied industrially in the field of
piezoelectric ceramics due to the high melting point and low toughness
values of ceramic materials. Therefore, the 3D printing of piezoelectric
ceramics has become a popular topic for research in the industry field
worldwide. This paper reviews recent research advances in 3D-printing
in the piezoelectric ceramics field to promote further breakthroughs in
this area. Followed by the introduction, the classification and charac-
teristics of the main 3D printing technologies, the piezoelectric ceramic
materials for printing, and the patterns of piezoelectric devices are sum-
marized in the piezoelectric ceramic field. Then, the working principles,
application areas, and research progress of each 3D technique are ex-
plained in detail. Finally, existing challenges are presented and future
opportunities are pointed out.
2. 3D printing piezoelectric ceramic method
To date, the main 3D printing methods for piezoelectric ceramics in-
clude and exclude lasers (Fig. 2), and the laser-based printing methods
include the stereolithography apparatus (SLA) and selective laser sinter-
ing (SLS) processes. SLA molding takes advantage of the characteristics
of photosensitive resins that rapidly cure under ultraviolet (UV) light
to form printing pastes [32]. The SLS uses a high-energy laser beam to
scan a powder bed surface, causing the powder to melt and adhere to
form the desired cross-sectional shape, followed by the placement and
sintering of the next powder layer; the powder layer is then stacked in
a layer-by-layer manner to form a three-dimensional component [33].
The printing method that does not feature a laser includes direct ink
writing (DIW) molding, inkjet printing (IJP) molding, and fused deposi-
tion molding (FDM). The DIW mold printing technology is either pneu-
matic or electric pressure, and the paste is extruded through a tiny inner
diameter needle to build a three-dimensional model in a cascading man-
ner [34]. IJP mold printing technology involves jetting ceramic ink in a
layer-by-layer manner to form a three-dimensional structure [35]. FDM
technology utilizes a mixture of thermoplastic resins and ceramic pow-
ders. The process involves melting the raw material into its fluid form,
extruding it to form fine filaments, and stacking the filaments [36]. The
laser-based printing method requires the installation of a light source
support structure; the light source moves from the bottom to the top to
complete a print job. Laser free-based printing does not require a light
source support structure, and the paste is printed by stacking the nozzles
in a layer-by-layer manner. Table 1 shows the comparison.
3D printing technology, as an emerging process, has contributed to
the development of piezoelectric ceramic devices to some extent. Table 2
compares the piezoceramic materials fabricated by 3D printing technol-
ogy and the conventional process. In general, piezoelectric ceramics fab-
ricated by 3D printing technology have lower piezoelectric properties
than those of the conventional process. However, in the work of Li and
Chen, the advantages of 3D printing technology in terms of electrical
properties are more obvious. In terms of density, the ceramic samples
prepared by 3D printing technology are generally lower than those by
the conventional process. This is mainly due to the addition of various
additives and grain size, which can be improved by additional process-
ing. Although there are differences between the two approaches, the
differences are small and within a reasonable range. 3D printing tech-
nology in the field of piezoelectric ceramics to improve the electrical
properties and sample density is also a major research direction in this
field in the future. Combined with the advantages of 3D printing tech-
nology in terms of printing accuracy and preparation cycle, 3D printing
technology has greater prospects for development. However, the small
amount of available printing materials limit the wide application of 3D

Table 1
Comparison of 3D printing technology.

Printing method Raw material status Molding order Resolutions Advantages Disadvantages

SLA Liquid Point 10 𝜇m Light curing molding has the Resin and equipment are expensive
characteristics of fast molding speed and
high surface quality
SLS Powder Point 80 𝜇m Material utilization rate close to 100% Rough surface quality due to powder heating and
melting molding
DIW Liquid Line 50 𝜇m Low cost without laser components Low mechanical strength of samples due to many
additives
IJP Liquid Surface 35 𝜇m No support structure required High uniformity of the ink preparation is difficult
FDM Filament Line 50 𝜇m The raw material is spool wire which is Print nozzle does mechanical movement, slow printing
easy to carry and replace speed

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D. Sun, Y. Lu and T. Karaki
Fig. 2. Classification of 3D printing technology [37–41].
Fig. 3. Major piezoelectric ceramic device types. (a) BT ultrasonic arrays[49]; (b) BT ultrasonic device with honeycomb structure[50]; (c) PMNT spherical ceramic
shell as ultrasonic transducer[43]; (d-f) PZT piezoelectric transducers; PZT monolithic ceramic actuator; PZT spiral actuator[51].
printing technology in the field of piezoelectric ceramics. At present,
the main systems of lead-free piezoelectric ceramics are BT, KNN, BCZT
and so on. Although there is a certain gap between the performance of
lead-based piezoelectric ceramics and lead-based piezoelectric ceram-
ics, lead-free piezoelectric ceramics are currently used in transducers
and sensors. Especially in recent years, the research on BT and KNN has
been increasing, so that their performance has been greatly improved.
Piezoelectric ceramic materials are mainly used as piezoelectric de-
vices in various mechanical devices. Currently, piezoelectric ceramic
devices are available in sheet, block, column, dot matrix and porous
shapes. Each printing technology uses its own characteristics to print
devices in different shapes. Chip and block devices are mostly printed
with light-curing printing technology. Column and dot matrix devices
are mostly prepared using inkjet printing techniques. Light-curing print-
ing, direct-write printing and selective laser sintering techniques can
be used to print porous structured piezoelectric ceramic devices. Fused
deposition techniques can be used to prepare piezoelectric ceramic de-
vices with multi-material layered structures. Cheng et al. [49] prepared
a 1.4 MHz focused ultrasound array by printing BT piezoelectric ce-
ramics using the SLA technique. The −6 dB bandwidth of the array is
40% and the insertion loss at the center frequency is 50 dB. The re-
sults show that the 3D printed BT ceramics have promising applica-
tions for complex shaped ultrasonic arrays. Zeng et al. [50] used the
Mask-Image-Projection-based Stereolithography (MIP-SL) technique to
prepare BT ultrasonic devices with complex structures. Upon testing,
the devices showed excellent material properties and output power.
Woodward et al. [43] printed (Mg1/3 Nb2/3 )O3 –0.35PbTiO3 (PMNT) hol-
low spherical shells using SLA technique for ultrasonic transducers. Sa-
fari et al. [51] used PZT material as the printing object and prepared
a variety of piezoelectric ceramic devices, including PZT piezoelectric
transducers, PZT monolithic ceramic actuator, PZT spiral actuator, etc
(Fig. 3).
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2.1. Laser-based processes
2.1.1. SLA
SLA is a rapid forming process that produces complex, small and
hollow components. This rapid forming process was developed by Hull,
an American researcher in 1986. In 1996, Griffith and Halloran first
proposed the application of light-curing molding technology to ceramic
manufacturing [52]. Since photosensitive resin is rapidly cured under
UV irradiation, one can add ceramic powder to photosensitive resin to
disperse the powder evenly in the solution through high-speed stirring;
this process prepares a printing paste with high estimated content and
low viscosity. A laser with a specific wavelength and intensity is fo-
cused onto the paste surface to make it solidify sequentially from point
to line and from line to surface to print one layer; then, the lifting ta-
ble moves the height of one layer piece vertically, curing another layer.
Layers are stacked to obtain a ceramic part blank [53–55] (Fig. 4a);
stacking is followed by a high-temperature degreasing process to ex-
pel organic components from the blank, and the final piezoelectric ce-
ramic part is obtained by sintering. Digital light processing (DLP) print-
ing technology is based on SLA technology; DLP differs from SLA be-
cause it uses a digital light source for shaping and printing the surface
(Fig. 4b).
For SLA printing technology, the printability of the paste is often a
key point; to ensure its printability, the paste is generally required to
have a low viscosity for flowability [56]. However, the solid content
of the paste should be high to ensure the curability of the paste and
the performance of the printed sample [45]. In addition, controlling the
printing accuracy is a key challenge of this technique.
At the beginning of the 21st century, French scientists Dufaudo, Mar-
chalp and others studied [57–59] the factors influencing the rheological
properties of lead-zirconate-titanate (PZT) suspensions; the researches
started, with a slurry configuration and found that the viscosity of the
D. Sun, Y. Lu and T. Karaki Resources Chemicals and Materials 2 (2023) 128–142

Fig. 4. Principle of light-curing printing. (a) SLA printing principle; (b) Schematic diagram of the different light sources used in DLP and SLA technologies.

Fig. 5. Influence of slurry viscosity and solid content on the density of printed samples. (a) The relationship between slurry viscosity and solid content [59]; (b)
Temperature dependence of viscosity for difffferent fifillers [60]; (c) SEM micrographs of SLA-printed BT ceramics prepared by various solid content slurries [59].

slurry increase with increasing solid phase content (Fig. 5a). Addition-
ally, the viscosity of the slurry was temperature dependent (Fig. 5b).
The application of stereolithography to chemical engineering and the
influencing factors of SLA molding accuracy have been investigated; in-
creasing the oxygen partial pressure of the solution improves the lateral
accuracy of molding. In 2019, Cheng et al. [60] prepared barium titanate
(BT) piezoelectric ceramics by SLA printing by mixing BT powders with
different mass fractions and photosensitive resins to form BT slurries
with solid contents of 70 wt.%, 75 wt.%, 80 wt.%, 82 wt.%, 84 wt.%,
and 86 wt.%. The printed samples were characterized, and the results
showed that the density is proportional to the slurry, and the density
of the samples reaches 5.68 g/cm3 when the solid content of the slurry
is 86 wt.%. The electrical properties were tested, and the study showed
that withhNL the increase in the BT solid content, the electrical proper-
ties of the ceramics increase significantly at 80 wt.% and then decrease
slightly, with the highest piezoelectric coefficient (d33 ) reaching 166
pC/N.
Unlike traditional methods of preparing piezoelectric ceramics, 3D
printing technology directly produces complex and highly accurate
piezoelectric ceramics and uses them as components in various devices.
The conventional light-curing molding method is an up-projection tech-
nique; however, this molding system has difficulty controlling the thick-
ness of a single-layer ceramic paste due to this drawback. Chabok et al.
[61] from the University of California have improved the light-curing
molding system by proposing the use of a down-projection light-curing
molding system to precisely control the layer thickness by improving the
accuracy of the vertical direction movement of the light-curing platform.
In addition, the curing paste is sealed between the printing platform and
the transparent container to reduce the oxygen-blocking effect gener-
ated by air; furthermore, this seal avoids problems, such as deformation
and warping, during printing. The printing of complex components of
PZT piezoelectric ceramics is realized. (Fig. 6b), and can be used as an
ultrasonic transducer in medical devices (Fig. 6a). In 2016, Chen et al.
[62] formulated a BT ceramic slurry with a solid content of 70 wt.% by
modifying the surface of BT powder; the researchers prepared a toroidal
piezoelectric ceramic array using the SLA printing method (Fig. 6c). It
can be used as an ultrasound transducer for energy focusing and ultra-
sound sensing. The relative density of the resulting sintered BT ceramic
sample is 93.7%, and the piezoelectric constant and relative dielectric
constant are 160 pC/N and 1350, respectively. On the basis of this ce-
ramic sample, relevant experiments were conducted on the piezoelec-
tric element prepared from this ceramic sample, and good results were
achieveda. In 2018, Chen et al. [42] used light-curing molding to print
PZT piezoelectric ceramics with solid content intervals ranging from

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D. Sun, Y. Lu and T. Karaki
Fig. 6. SLA printing technology directly prints complex piezoelectric ceramic devices. (a) Complex piezoelectric ceramic devices for medical applications; (b)
Ultrasonic transducer array printed by SLA technology [61]; (c) Ring-shaped piezoelectric ceramic arrays prepared by SLA printing method [62].
Fig. 7. Various piezoelectric ceramic devices printed by DLP technology. (a) Complex-structured BT ceramics [63]; (b) Porous structure of BT ceramics and samples
with different porosity [64]; (c) Transducer devices [65].
78% to 89%. These piezoelectric ceramics perform best when the solid
content is 81.8%, with a piezoelectric constant d33 of 300 pC/N, a di-
electric constant of 765, and a dielectric loss of 0.020. In addition, a
two-dimensional ultrasonic transducer array has been designed and de-
veloped on this basis. A total of 81.8% of the slurry produces an array
with a 35% bandwidth of −6 dB, which is similar to conventional PZT
ceramic transducers (∼31% bandwidth), demonstrating the high poten-
tial of applications of 3D-printed PZT ceramics.
The evolution of the SLA printing process is the DLP process, and the
DLP and SLA printing principles are the same. The difference between
these techniques is that the light source used in DLP is digital and used
directly on the surface molding; this difference greatly improves the
printing efficiency. Regarding the printing sample surface quality and
molding rate, DLP has certain advantages. As with SLA technology, there
are many factors affecting DLP printing, such as the slurry solid content,
the sintering temperature, and the preconditioned slurry powder parti-
cle size.
In 2021, Liu et al. [63] developed a DLP technique for 3D printing
BT piezoelectric ceramics. Acryloyl morpholine (ACMO) with a high re-
fractive index was selected as a photosensitive monomer and used to
construct a BT paste with a high solid content, low viscosity, and high
curability. By reducing the exposure time of a single layer, the mold-
ing efficiency is greatly improved. Several experiments have been con-
ducted with BT slurries in the solid content range of 65 wt.% to 82 wt.%,
among which the BT ceramics prepared with 80 wt.% slurry have the
best performance levels, with piezoelectric constants of 168.1 pC/N. Ce-
ramics for octet truss and gyroscope structures have been prepared us-
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ing the above optimal process parameters (Fig. 7a), and the feasibility
of the process in forming complex structures has been verified. Finally,
the ceramic has been assembled into a hydrophone, and the hydroa-
coustic function has been successfully demonstrated. This finding has
important implications for the future design and fabrication of piezo-
electric ceramic matrix composites for functional devices. In 2021, Jiang
et al. [64] successfully prepared a series of BT piezoelectric ceramic
porous scaffolds using DLP printing technology (Fig. 7b). Different tem-
peratures were selected for sintering to obtain high-precision and high-
purity samples, and the optimal sintering temperature was determined
to be 1425 °C. The BT scaffolds with different porosities were tested; the
compressive strength and d33 gradually decrease as the scaffold poros-
ity increases from 10% to 90%, indicating that any desired mechanical
and electrical properties are obtainable by adjusting the porosity. Chen
et al. [65] have prepared BaTiO3 lead-free piezoelectric ceramics using
DLP (Fig. 7c). The researchers investigated the performance levels of ce-
ramic components using ceramic powders with particle sizes of 200 nm,
500 nm, and 600 nm as raw materials for ceramic slurry;the researchers
concluded that the particle size of ceramic powder is a key factor af-
fecting the performance levels of sintered ceramic components. Subse-
quently, the effects of particle size on the rheological properties, pho-
topolymerization behaviors, on the densities, particle sizes, and piezo-
electric and dielectric properties of the suspensions were investigated.
The particle size has a significant effect on the depth of cure of ceramic
suspensions. As the average particle size decreases, the number of scat-
tering centers increases, the diffuse reflectance increases and the diffuse
transmittance decreases, leading to a decrease in the depth of cure. The
D. Sun, Y. Lu and T. Karaki
Fig. 8. Principle and molding process of SLS printing technology.
d33 value increases with increasing grain size, reaching 206 pC/N at
875 nm.
SLA molding can be used to manufacture parts with complex struc-
tures and high precision requirements; this process can be performed
at room temperature and ambient pressure. The disadvantage of SLA
molding is that the photosensitive resin is slightly toxic and pollutes the
environment to a certain extent. SLA molding is a high-cost process that
requires a large amount of raw materials; additionally, it requires a cer-
tain environment for experimentation, which must be conducted under
the circulating air and dim light.
2.1.2. SLS
SLS was proposed and patented by Deckard [66], a graduate student
at the University of Texas, in 1986. SLS technology uses a high-intensity
infrared laser as the light source. The powder material laid flat on the
printing platform is preheated to a temperature slightly below the melt-
ing point and scraped flat with a squeegee, and the cross-sectional shape
of the blank to be printed is first scanned on the powder plane with ei-
ther a CO2 laser or a Nd:YAG laser; afterward, the area is irradiated
with infrared light, and the powder in the cross-sectional area is sin-
tered together to form a blank cross-section. Then, a new layer of pow-
der material is laid on and selectively sintered in a continuous cycle,
stacking in a layer-by-layer manner to form a three-dimensional part
[67] (Fig. 8). There are two types of SLS processes—indirect selective
laser sintering (iSLS) [68] and selective laser melting (SLM) [69] de-
pending on whether a binder is used during manufacturing. Indirect
SLS technology uses polymer binders therefore, subsequent processing,
such as degreasing and sintering, is required to densify ceramic compo-
nents. Depending on the laser power used, direct SLS technology can the
promote partial or complete melting of ceramic particles, enabling the
direct integration of powder molding and sintering; this action elimi-
nates the need for subsequent processing, resulting in denser printed
blanks and saving material.
Most of the existing studies on selective laser sintering involve
direct molding methods; these methods are being developed in the
field of piezoelectric ceramics, which are preferential techniques for
preparing piezoelectric ceramic samples. However, the materials used
in the piezoelectric ceramics prepared by SLS technology are mostly
composite materials. Kuznetsov et al. [70] prepared PZT+SiO2 func-
tionally graded piezoelectric ceramics using SLS printing technology
(Fig. 9a). In this material can be used to fabricate smart devices.
Shuai et al. [71] successfully used polydopamine functionalized hy-
droxylated BT nanoparticles homogeneously dispersed in PVDF scaf-
folds prepared by SLS technique(Fig. 9b), which significantly enhanced
the generated voltage, and the piezoelectric effect generated by this
scaffold plays an important role in restoring bone tissue. And the ten-
sile strength and modulus of the scaffold were also significantly en-
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Resources Chemicals and Materials 2 (2023) 128–142
hanced. This scaffold has great potential for application in bone re-
generation. Qi et al. [72] used a new method of applying solid-state
shear milling, melt blending and low-temperature grinding techniques
for large-scale and non-solvent production of functional nanocompos-
ite powders. Polyamide 11 (PA11)/BaTiO3 nanocomposite powders for
SLS technology were successfully prepared. A method was provided
for the large-scale production of functional nanocomposite powders.
High-precision PA11/BT nanocomposites were successfully prepared by
printing this powder using SLS technology (Fig. 9c). It was successfully
demonstrated that the nanopowders prepared by this technique signif-
icantly increased the sintering window of PA11/ BT nanocomposites
(from 10.1 to 14.6 °C) and that the dielectric constant and piezoelec-
tric coefficient of PA11/BT nanocomposites increased after solid-state
shear milling treatment. Tarasova et al. [73] successfully prepared 3D
samples from PVDF+PZT, SiO2 , and PZT powders by a selective laser
sintering process and explored the important factors affecting SLS print-
ing: laser type and power, scanning speed, and spot diameter. Using
this technique, Gureev et al. [74] have synthesized and sintered PbO,
ZrO2 , and TiO2 raw powders, explored the conditions of selective laser-
induced sintering of the mixtures, obtained different phase structures
by adjusting the laser power, derived laser treatments for obtaining PZT
ceramic products immediately during sintering or afterward with ad-
ditional annealing, and finally obtained PZT ceramic masses with ap-
proximately 20% of the theoretical density. Due to the low density,
the prepared PZT ceramics are sparse, porous and very easy to break.
This study demonstrates the possibility of obtaining bulk PZT ceramic
products from a stoichiometric mixture of lead, zirconium and titanium
oxide. This study shows that the magnitude of laser power determines
the density of the printed sample, and the power is proportional to the
density. Shishkovsky et al. [75] have chosen a Nd:YAG laser of ≤25 W
and prepared PZT piezoelectric ceramics by SLS printing technology.
Due to the use of a lowpower laser, some ceramic particles are not
completely melted, and the prepared blanks are high-porosity blanks
with low densities. Sheldon A. et al. [76] developed a new 3D mold
printing technology with SLS: laser engineering mesh forming technol-
ogy (LENSTM). This technique allows the fabrication of PZT directly
on metal structures for use as sensors. Using a 500 W Nd:YAG laser, a
crack-free PZT piezoelectric ceramic with a relative density of 90% is
prepared on a stainless steel substrate by coaxially feeding the powder
(Fig. 9d). LENSTM-treated bulk PZT samples have bulk densities of 90%
of the theoretical density of the PZT parts processed by LENSTM due
to the high thermal stress and excessive evaporation and combustion
of the PZT powder. The ability to directly fabricate porous and dense
PZT structures provides a wide range of potential applications for this
process.
SLS is a type of laser forming process, and it requires equipment
support. Parts can be used directly after printing without additional
D. Sun, Y. Lu and T. Karaki
Fig. 9. Piezoelectric ceramic parts prepared by SLS technology. (a) PZT+SiO2 functionally graded piezoelectric ceramic samples [70]; (b) LENSTM processed bulk
net shape PZT compacts on 316 L stainless steel substrate [76]; (c) Objects printed by SLS using the solid state shear milling treated PA11/BT nanocomposite powders
with various BT particle loading [72]; (d) PVDF/BT composite scaffold [71].
sintering or curing. However, the preparation of piezoelectric ceram-
ics by selective laser sintering is still in its infancy, mainly due to the
strict requirements of the printing material. The material is limited to
the powder form without a liquid medium; therefore, it is difficult to
mix the raw materials well with each other before starting the process.
To date, this technology is mainly used for functional ceramics, such
as Al2 O3 and ZrO2 , with high market maturity. It is difficult to grasp
the influences of laser power and other parameters on the structures
and performance levels of piezoelectric ceramics, and the preparation
of piezoelectric ceramics has high requirements for raw materials and
equipment. Piezoelectric ceramics prepared by laser-selective sintering
technology have poor densities and low molding accuracy, which make
it difficult to meet practical application requirements.
2.2. Laser-free processes
2.2.1. DIW
DIW, a typical ceramic additive manufacturing technique, is a mold-
ing method in which a ceramic suspension is extruded and cured by
pumping pressure through a fine needle and by stacking in a layer-by-
layer manner into a blank by computer-controlled alignment molding
(Fig. 10). This technique is a simple, adaptable method for a wide range
of materials, such as ceramics (monolithic and composite), polymers,
alloys and food products [77]. DIW technology was first introduced in
1997 by J Cesarano [78] in the USA, and it was first applied to the field
of ceramics. This method has fewer restrictions than other methods on
the type and quantity of printing materials, and it can realize multimate-
rial printing [79]. As with most ceramic additive technologies, a key part
of direct-write forming technology is the configuration of the ceramic
slurry. The slurry should be homogeneous, and clumps and bubbles must
be removed to obtain fine prints [80]; the slurry should have a high solid
content, low viscosity, good viscoelasticity, and flow through the noz-
zle at a relatively low pressure. The size of the nozzle is a key factor
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Resources Chemicals and Materials 2 (2023) 128–142
affecting the printing effect in direct-writing molding technology. Gen-
erally, to improve the resolution of the print, a smaller diameter nozzle
is chosen; however, the smaller the diameter is, the greater the extru-
sion pressure and the larger the printing time. Therefore, the pressure
should be selected to match the print material nozzle size to ensure the
smoothness of the print and the print resolution.
Due to the flexibility of the process and the variety of materials that
can be printed, direct-to-shape printing technology is used relatively of-
ten in practical production processes. This technology is used to manu-
facture piezoelectric ceramics. After continuous developments, the pow-
der, paste, additives, sintering temperature and printing equipment are
analyzed and improved to obtain the best finished piezoelectric ceram-
ics.
PZT piezoelectric ceramics were first prepared by Tuttle and Smay
et al. [82,83] using a direct-write-forming printing technique. Among
these ceramics, the piezoelectric constants and electromechanical cou-
pling coefficients of direct-written printed bulk PZT are similar to those
of the control sample prepared by cold isostatic pressure; the measured
dielectric constants (1 Hz) are 831 and 1081, and the corresponding d33
values are 388 and 496 pC/N, respectively, when PZT is printed into lin-
ear and toroidal shapes using needles of different sizes (Fig. 11a,b). Li
et al. [84] investigated a new organic suspension for PZT printing and
fabricated complex unbranched structured PZT products by DIW pro-
cess (Fig. 11c). The printed green valve body can be flexibly deformed
and with a good heating process, the actual density of the ceramic sin-
tered body can reach more than 98% (Fig. 11d), and the ceramic sintered
body has good piezoelectric properties with an average d33 of 265 pC/N.
The technology is simple, with low processing cost, and is an attractive
method for manufacturing piezoelectric ceramic products with complex
structures, solving the key problems in existing ceramic additive manu-
facturing technology. Kim et al. [85] have prepared a dense bulk BaTiO3
piezoelectric ceramic material using direct-write molding. The maxi-
mum density of the printed BaTiO3 piezoelectric ceramics is 3.93 g/cm3 ,
D. Sun, Y. Lu and T. Karaki
Fig. 10. DIW printing principle and printing equipment. (a) The main steps of the DIW printing process [81]; (b) Experimental set-up for the DIW process[44].
Fig. 11. (a,b) Optical micrographs of as-dried and sintered PZT arrays [82]; (c) DIW technology prints 3D woodpile structure scaffold and SEM image of sintered
sample [84].
which is 65.3% of the theoretical density, by adjusting the ratio of the
binder and making other changes. The analysis was performed for dif-
ferent sintering temperatures; the BaTiO3 piezoelectric ceramics sin-
tered at 1400 °C have the highest grain growth tendency, and the piezo-
electric and dielectric constants are 200 pC/N and 4730, respectively,
at 1000 Hz. Direct-write printing has the potential for the mass pro-
duction of bulk piezoelectric ceramics. In 2020, Wang et al. [86] suc-
cessfully prepared a lead-nickel-niobate–lead-zirconate-titanate (PNN–
PZT) piezoelectric ceramic composite with high electromechanical cou-
pling and pressure sensitivity using a homemade dual-nozzle 3D printer,
which allows the preparation of arbitrary mesh shapes by design. The
selection of a polydimethylsiloxane (PDMS) elastic matrix composed
of a flexible ceramic polymer composite and doped with an Ag-coated
PNN–PZT (0.55Pb(Ni1/3 Nb2/3 )O3 –0.135PbZrO3 –0.315PbTiO3 ) ceramic
heterojunction particles. The 3D printed lattice composite doped with
ceramic particles is more flexible and has a piezoelectric coefficient
reaching 400 pC/N. Without using a charge storage capacitor, 20 light-
emitting diodes (LEDs) can be operated simultaneously with a force of
20 N. The lattice has good piezoelectric properties, and its flexibility
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Resources Chemicals and Materials 2 (2023) 128–142
and tensile properties can potentially replace brittle ceramic ceram-
ics; additionally, the materials have great potential for as applications
in soft robots, artificial muscles, and biological signal recognition. Li
et al. [87] prepared potassium sodium niobate (KNN) piezoelectric ce-
ramic scaffolds with different structural parameters using Li, Ta, and Sb
parametrized into KNN powder; the resea rchers conditioned the pow-
der as a piezoelectric ink and printed models by direct writing into a
shape. The samples were sintered at 1050 °C, 1100 °C and 1130 °C for
2 h and observed by electron microscopy; the results show that the sam-
ples sintered at 1100 °C are in good agreement with the original pow-
der, indicating that no significant phase change occurs during sintering.
The composition, microstructure and piezoelectric parameters of the sin-
tered samples were observed. The relative density reaches 98%, d33 is
280 pC/N, the dielectric constant 𝜀 is 1775, the residual polarization
strength Pr is 18.8 𝜇C/cm2 , and the coercivity field Ec is 8.5 kV/cm.
Although direct ink writing printing can produce piezoelec-
tric ceramics with excellent performance, it is always a com-
mon goal for researchers to further improve the performance of
piezoelectric ceramics. In 2004, Y. Saito et al. [88] fabricated
D. Sun, Y. Lu and T. Karaki Resources Chemicals and Materials 2 (2023) 128–142

Fig. 12. DIW technology for the preparation of textured ceramics. (a) Model of baffled nozzle; (b) Electron microscopy image of BT template in cross section of
sintered sample; (c) Lotgering factor as a function of position (position/diameter) for filaments printed at various printing rates with different aspect ratio [89].

(K0.44 Na0.52 Li0.04 )(Nb0.84 Ta0.10 Sb0.06 )O3 textured ceramics by the re-
active template grain growth (RTGG) method, which triggered an up-
surge in high-performance piezoelectric ceramics fabrication. Yet even
today, RTGG remains the most valuable method for preparing textured
ceramics. However, textured ceramics are still not realized in industrial
production due to the complexity of the process and the long prepara-
tion cycle. With the rise of 3D printing, the idea of using 3D printing to
prepare textured piezoelectric ceramics has been gradually realized by
researchers. Walton et al. [89] have used the DIW printing technique
to produce lead Pb(In1/2 Nb1/2 )-Pb(Mg1/3 Nb2/3 )O3 -PbTiO3 ) (PIN-PMN-
PT) multifunctional piezoelectric ceramics, in which BT flake powder
is chosen as the template powder. This printing is characterized by the
improvement in the nozzle of the printing device by introducing a baf-
fle at the nozzle, generating lateral shear force when the slurry flows
through the nozzle (Fig. 12a); additionally, it achieves the orientation
of the template powder inside the slurry by the shear effect of the noz-
zle (Fig. 12b), thus producing a high-performance woven piezoelectric
ceramic. It was found that the volume of material aligned during the
printing process increases with increasing nozzle aspect ratio and print-
ing rate (Fig. 12c).
DIW forming technology is a common process in the field of piezo-
electric ceramic additives. The advantages of DIW are that it does not
require external conditions, such as lasers and UV light, the process is
simple and low cost, it can be performed in a room temperature en-
vironment, and the ceramic powder is uniformly and stably dispersed
in the slurry; this phenomenon ensures the density of the sample. How-
ever, the size of the powder and the solid content of the slurry should be
controlled during preparation to ensure that the slurry can be extruded
smoothly. However, the slurry contains different additives, such as sur-
factants, dispersants and binders, which may lead to the formation of

136
D. Sun, Y. Lu and T. Karaki
Fig. 13. Principle of IJP printing technology and two types of inkjet mechanisms.
various defects in the final part after sintering. These defects are related
to the removal of binders and additives that lead to volume shrinkage
and crack formation in the final 3D printed part, resulting in densifica-
tion and poor mechanical strength [90], which are issues that must be
addressed in the existing direct-write forming technology.
2.2.2. IJP
In the field of ceramics, IJP is mostly used for ceramic printing, which
plays a decorative role; IJP is a common printing technology in indus-
trial production to date. Ceramic powders are mostly used as pigments
to be combined on the surfaces of organic carriers by inkjet printing.
Inkjet molding 3D printing has evolved from the layer-by-layer super-
position of flat shapes into a solid. Inkjet printers are mainly divided
into two modescontinuous-jet and drop-on-demand to form air pressure
pulses to achieve the on-demand spraying of droplets. In the drop-on-
demand mode, the nozzle is divided into two mechanisms—heating jet
and piezoelectric jet—and then controlled by a computer to achieve
slurry jet molding in a preset area [91] (Fig. 13). In the 1990s, the tech-
nology of preparing ceramics using ink-jet printing technology emerged,
mostly with ZrO2 and TiO2 ceramics [92,93]. To date, inkjet printing
technology is widely used in solar cells [94,95], sensors [96,97], elec-
tronic circuits [98,99] and other fields. A key step in inkjet printing
and molding technology is the preparation of ceramic ink; a mixture of
ceramic powders, binders, and other organic additives are formulated.
Ceramic inks require suitable viscosity, surface tension, electrical con-
ductivity, high solid content, and fast drying rate values. In addition, the
printing results depend on the setting of various printing parameters.
Derby B et al. [100] have conducted experiments on the prepara-
tion of PZT piezoelectric ceramics by multigroup inkjet printing using
an azeotropic mixture of methyl ethyl ketone and anhydrous ethanol
(MEK/EtOH) (67/33 wt.%) as a medium, and the two types of PZT
suspensions are experimentally investigated by direct inkjet printing
at 25 °C and 120 °C, respectively. The effects of processing parame-
ters, such as mixing time and temperature, on the optimization of vi-
able jet viscosity are investigated. This investigation is followed by a
study of the dispersant and solvent composition to produce an inkjet-
ready Pb(Zr0.53 Ti0.47 )O3 (PZT)−5H powder suspension with a solid con-
tent reaching 40 vol.%. The powder suspension is made with a 35%
PZT suspension. These are sintered to full density, with less than 1%
porosity and no significant distortion (Fig. 14a). At the beginning of the
21st century, R. Noguera’s team [101,102] have realized the printing of
a series of micro-PZT columns with resolutions reaching 50 𝜇m using a
piezoelectric-driven drop-on-demand IJP technique with a 10 vol.% PZT
solution. The influencing factors related to the preparation of the sus-
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Resources Chemicals and Materials 2 (2023) 128–142
pension, the driving parameters of the print head, and the diameter and
height of the columns to prepare the microcolumn array structures are
explored. After sintering, the ceramic micropillars are dense (Fig. 14b),
and these structures greatly improve the performance levels of imaging
probes with 1–3 ceramic polymer composites and the performance lev-
els of microdeformation mirrors for optical adaptive systems, which are
more widely used in ultrasonic transducers and thus improve the spa-
tial resolution of ultrasound probes. Inkjet printing is used in the field
of lead-based piezoelectric ceramics and has been studied for lead-free
piezoelectric ceramics. Wagata et al. [103] have used BT precursor so-
lution for IJP for preparing a BT pattern. Unlike the conventional IJP
method, this ink-jet technique uses a precursor solution deposited on
a heated substrate, which fundamentally avoids the occurrence of hole
plugging. The ceramic precursors are deposited by an inkjet at 360 °C
and then heat-treated at 650 °C for 4 h to prepare a crystalline BT dot
matrix. The size and height of a dot are controlled by adjusting the con-
centration of the solution and the number of droplets. In addition, the
researchers prepare dot arrays of different diameters by controlling the
droplet concentration and volume (Fig. 14c).
Similar to inkjet printing is binder jetting. Unlike inkjet printing,
binder jet technology uses an inkjet print head to spray an adhesive onto
the powder, bonding layers of powder in a selected area. Each layer of
powder is combined into one by the penetration of the binder. Stacking
in this manner creates a three-dimensional structure of the object. The
binder jetting technology has the advantages of a simple manufacturing
method, no material size restriction, and high practicality, which is suit-
able for the manufacturing of amorphous devices [104]. Gaytan et al.
[105] have prepared BT ceramics for use as ceramic capacitors and sen-
sors using the binder jetting technology and modified the build param-
eters and sintering profiles to optimize the obtained density and crystal
structure. Printed samples were obtained at densities of 3.93 g/cm3 ,
d33 values of 74.1 pC/N, and relative permittivity values of 8.6–6.23
at frequencies ranging from 12.4 to 18 GHz. By studying the binder
dose and the sintering temperature, it was concluded that the density
of the sintered sample is inversely proportional to the binder saturation
and inversely proportional to the sintering temperature. Sufifiiarov et al.
[106] prepared barium titanate piezoelectric ceramic samples using the
binder jetting technology, and two initial powders with different grain
size distributions were investigated. The influence of the sintering pro-
cess and the grain size distribution of the raw material on the grain size
and functional properties was investigated. After the experiments, the
piezoelectric coefficient of the fine unimodal powder sample was 183
pC/N, which was greatly higher than that of the coarse unimodal pow-
der (118 pC/N). The effect of binder saturation on the sintering pattern
D. Sun, Y. Lu and T. Karaki
Fig. 14. Various complex structures of piezoelectric ceramic prepared by IJP printing technology. (a) Stroboscopic image of a PZT suspension being delivered by a
single ink-jet printhead and images of printed objects from green body to sintered ceramics [100]; (b) PZT piezoelectric array [101]; (c) Laser microscopic images
of BT dot patterns [103].
is also tested. Schult et al. [107] studied the printing of porous barium
titanate ceramics. It was found that as the size of the powder increased,
the binder saturation inside the blank decreased and the volume shrink-
age after sintering also decreased significantly. However, binder jetting
is not actually widely used in the piezoelectric ceramics field due to its
low resolution, low accuracy, and low printing efficiency. Stability is not
guaranteed due to the easy clogging of the binder, the inhomogeneous
stresses generated by the nozzle, and the easy appearance of cracks be-
tween the layers. This also limits the development of such methods in
the piezoelectric ceramics community. Huang et al. [108] proposed an
inorganic colloidal binder that can solve the problems of nozzle clogging
and particle settling. Inorganic colloidal binders have also been used to
successfully print zirconium dioxide ceramic parts. As a breakthrough
in binder injection, it also provides new ideas for the extension of this
technique in the piezoelectric ceramics field.
IJP forming does not require the assembly of a support structure, and
the forming process is directly cured and formed without laser technol-
ogy. Moreover, inkjet printing has advantages regarding printing costs,
and it is simpler and more effective than traditional processes in terms
of shape and accuracy control [109]. The technical difficulties of inkjet
molding lie in the configuration of the printing paste. Due to the addi-
tion of various additives in the paste, the uniformity of the paste density
must be ensured to guarantee the densities of the printed blanks. In ad-
dition, it is necessary to ensure that the fineness of the powder in the
slurry matches the size of the printhead; otherwise, it is easy to cause
nozzle blockage and interrupt printing.
2.2.3. FDM
FDM is a process successfully developed by the American scholar
Dr. Scott Crump [110] in 1988; after continuous processing and mod-
ification, FDM has become a common additive manufacturing method.
The raw material is a hot-melting filamentary material, which is intro-
duced into the nozzle with a mechanical device; the material is heated
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and melted into a semiliquid state inside the nozzle and moves accord-
ing to a trajectory set by a computer. Additionally, the viscous forming
material and support material are selectively coated on the table, and
the cross-sectional profile forms after rapid curing. After the first layer
forms, the nozzle rises to a specific height for the next layer of coating,
and the layers are stacked to form a three-dimensional product (Fig. 15).
The ambient temperature of the table housing must be controlled dur-
ing the process. Initially, FDM molding technology was mostly applied
to the deposition processes of plastic objects, and it was difficult to use
for advanced ceramics and metals [111]. With continuous research on
deposition processes, examples of ceramic preparation using FDM tech-
nology have gradually emerged.
At Rutgers University, USA, Danforth S C et al. [112] have patented
the first fusion deposited ceramic (FDC) technique for FDM technology.
In this method, polymers are premixed with ceramic powders. The ce-
ramic particles are used to form thin filaments drawn from a spool and
fed into a heated extruder nozzle that follows a computer-set route to ob-
tain the final printed model. A. Safari et al. [113] successfully printed
PZT piezoelectric ceramics using FDC, with a sample having a d33 of
397 ± 16 (pC/N). The sample has a strong bond between the printed
layers, and the sintered relative density of the fabricated parts reaches
95%. At the beginning of the 21st century, Fafari. A. et al. [114] im-
proved the conventional FDM device and successfully developed a mul-
timaterial deposition system (FDMM) with a multilayer PZT design in-
cluding two different piezoelectric electroactive materials (soft PZT and
hard PZT) deposited in a layer-by-layer manner with a layer thickness
of 250 μm (Fig 16a). No defects are observed at the interface of hard
PZT and soft PZT by electron microscopy (Fig 16b). In addition, a mul-
tilayer piezoelectric element transducer is also printed (Fig 16c). In this
structure, each layer is adjacent to each other and spaced 76 𝜇m apart.
On the next layer, it’s a different material. This structure can rotate in
the X and Y directions. It provides a new idea for the printing of com-
plex transducer. Most of the existing prints on piezoelectric ceramics
D. Sun, Y. Lu and T. Karaki
Fig. 15. Principle of FDM printing technology.
Fig. 16. (a) Multimaterial deposition equipment for FDM printing technology [116]; (b-c) Multi-material multilayer piezoelectric transducer and sensor fabricated
by FDM printing technology [114].
are PZT-based. In the field of lead-free piezoelectric ceramics, Kim et al.
[115] have printed barium titanate/polyvinylidene fluoride (BT/PVDF)
nanocomposites using FDM technology. The nanocomposite combines
the functional properties of barium titanate (piezoelectric, pyroelectric
and dielectric) with the flexibility and lightness of polyvinylidene flu-
oride. The electrical properties are investigated, and the piezoelectric
coefficient of the thermally polarized nanocomposite is determined to
be three times higher than that of the solvent-cast nanocomposite with
a d33 of 21 × 10−3 (PC/N), which is a 2.3-fold increase relative to the
solvent-cast nanocomposite. This increase implies that the 3D printing
process has a great impact on the piezoelectric properties, as it provides
uniform dispersion, reduces porosity and cracking, and mitigates the
agglomeration of BT nanoparticles.
Fused deposition molding does not require laser assistance and can
be directly cured into a shape, with low cost, no environmental pol-
lution, and easy and fast post maintenance. When building a model,
it is usually necessary to design an auxiliary support structure, and
the support structure must be processed after printing. In the field of
piezoelectric ceramics, there are few piezoelectric ceramic filaments on
the market; therefore, researchers to date are working on fused depo-
sition molding using composite materials to achieve the same perfor-
mance as piezoelectric ceramics. Additionally, the printing accuracy of
fused deposition is lower than that of other printing methods, and the
surface streaks of the formed parts are more obvious. Since the fila-
ments are stacked in a fused state, the bonding forces between the lay-
ers are limited, resulting in a weak structural strength in the thickness
direction.
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3. Outlook
3D printing is an efficient and fast molding method with great
prospects in the field of piezoelectric ceramics; 3D printing processes
can achieve high-precision and high-efficiency molding. However, the
existing 3D printing processes of piezoelectric ceramics are in their ini-
tial stages. There are many difficulties to overcome in the future, and
many innovations and challenges must be explored. Many problems and
challenges bring new opportunities for the development of 3D printing
in the field of piezoelectric ceramics. In the future, the development
direction will mainly focus on the following aspects:
1) An important factor for piezoelectric ceramic printing is to ensure
that the ceramic slurry has a high solid content and low viscosity.
Therefore, it is necessary to add dispersants, binders and other or-
ganic additives to the slurry configuration process, leading to many
problems in degreasing, such as an excessively long degreasing time,
easily appearing pores inside the sample, sample deformation and
lack of density. Therefore, to ensure the performance of the samples,
the addition of organic additives should be minimized, and research
on binders and dispersants should be strengthened to improve their
stability and dispersibility characteristics.
2) Regarding ceramic properties, although some of the piezoelectric ce-
ramic samples manufactured by 3D printing reach an ideal state,
most samples fail to achieve the intrinsic properties and must be
improved concerning their paste configuration, process, etc.; by im-
proving the properties,the printed samples can reach their ideal per-
D. Sun, Y. Lu and T. Karaki
formance levels. It is possible to improve the performance levels of
piezoelectric ceramics by modifying them. In recent years, research
on the weaving of piezoelectric ceramics has gradually increased,
and high-performance multisystem piezoelectric ceramics are one
of the future research directions for the directional arrangement of
the internal grains of piezoelectric ceramics to obtain better perfor-
mance levels.
3) The existing 3D printing piezoelectric ceramic objects are mostly
lead-based piezoelectric ceramics; although high-performance piezo-
electric ceramics can be obtained, lead is a toxic element. There
are many environmental and human health hazards resulting
from the preproduction, use and post processing of these mate-
rials;therefore,the printing research on lead-free piezoelectric ce-
ramics should be increased. Improving the performance levels of
lead-free piezoelectric ceramics can be achieved through high-
performance and high-efficiency processing; this action should be
performed in more areas to replace lead-based piezoelectric ceram-
ics. To date, the 3D printing of barium titanate and potassium sodium
niobate piezoelectric ceramics has been studied, and certain results
have been achieved. Through continuous research, the performance
levels of lead-free piezoelectric ceramics will hopefully reach those
of lead-based piezoelectric ceramics and be widely used in the near
future.
Declaration of Competing Interest
We declare that we have no financial and personal relationships with
other people or organizations that can inappropriately influence our
work, there is no professional or other personal interest of any nature
or kind in any product, service and company.
Fundings
This work was financially supported by the Scientific Research Fund-
ing Project of the Educational Department of Liaoning Province in 2020,
grant number LQ2020008.
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