Journal of the European Ceramic Society xxx (xxxx) xxx–xxx

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Journal of the European Ceramic Society

journal homepage: www.elsevier.com/locate/jeurceramsoc

Review article

3D printing of ceramics: A review

Zhangwei Chen , Ziyong Li, Junjie Li, Chengbo Liu, Changshi Lao , Yuelong Fu, Changyong Liu,
⁎ ⁎

Yang Li, Pei Wang, Yi He

Additive Manufacturing Institute, College of Mechatronics and Control Engineering, Shenzhen University, Shenzhen, 518060, China

ARTICLE INFO ABSTRACT

Keywords: Along with extensive research on the three-dimensional (3D) printing of polymers and metals, 3D printing of
3D Printing ceramics is now the latest trend to come under the spotlight. The ability to fabricate ceramic components of
Ceramics arbitrarily complex shapes has been extremely challenging without 3D printing. This review focuses on the latest
Feedstock advances in the 3D printing of ceramics and presents the historical origins and evolution of each related tech-
Sintering
nique. The main technical aspects, including feedstock properties, process control, post-treatments and energy
Applications
source–material interactions, are also discussed. The technical challenges and advice about how to address these
are presented. Comparisons are made between the techniques to facilitate the selection of the best ones in
practical use. In addition, representative applications of the 3D printing of various types of ceramics are sur-
veyed. Future directions are pointed out on the advancement on materials and forming mechanism for the
fabrication of high-performance ceramic components.

1. Introduction manufacturing technologies used to fabricate physical parts in a dis-

Owing to their various excellent properties, ceramics are used in a
wide range of applications, including the chemical industry, machinery,
electronics, aerospace and biomedical engineering. The properties that
make them such versatile materials include high mechanical strength
and hardness, good thermal and chemical stability and viable thermal,
optical, electrical and magnetic performance. Ceramic components are
generally formed into the desired shapes starting from a mixture of
powder with or without binders and other additives, using conventional
technologies, including injection moulding, die pressing, tape casting,
gel casting etc. [1]. Sintering of the green parts at higher temperatures
is further required to achieve densification. However, these ceramic
forming techniques give rise to limitations in terms of long processing
times and high cost. Structures with highly complex geometries and
interconnected holes are impossible to produce as moulding is usually
involved in these techniques. On the other hand, machining of ceramic
components tends to be extremely difficult owing to their extreme
hardness and brittleness. Not only are the cutting tools subject to severe
wear, but defects such as cracking might also be generated in the
ceramic parts, not to mention the difficulty of achieving good surface
quality and dimensional precision.
The emergence of three-dimensional (3D) printing technologies,
also referred to as additive manufacturing (AM), is regarded as a
manufacturing revolution. 3D printing is a series of advanced
crete point-by-point, line-by-line or layer-by-layer additive manner
from 3D CAD models that are digitally sliced into 2D cross sections. 3D
printing is a unique manufacturing philosophy that enables the flexible
preparation of highly complex and precise structures that are difficult
to realise using traditional fabrication methods such as casting and
machining [2]. Productivity can also be significantly increased as many
objects can be built in a single run. As a result, 3D printing has rapidly
gained attention across the science and engineering communities since
its emergence in the 1980s.
The introduction of 3D printing into the manufacturing of ceramic
components offers entirely new possibilities for addressing the above-
mentioned problems and challenges. The 3D printing of ceramics was
first reported by Marcus et al. [3] and by Sachs et al. [4] in the 1990s.
To date, with the latest advances in materials science and computer
science, a great variety of 3D printing technologies have been specifi-
cally developed for ceramic manufacturing. According to the form of
the pre-processed feedstock prior to printing, these technologies can
generally be categorised into slurry-based, powder-based and bulk
solid-based methods, as summarised in Table 1. Note that slurry-based
technologies use ceramic/polymer mixtures with viscosities ranging
from low-viscosity (∼mPa·s) inks with a low ceramic loading (up to
30 vol%) to high-viscosity (∼Pa·s) pastes with a much greater ceramic
loading (up to 60 vol%).
This review aims to discuss the state of the art with regard to the

⁎
Corresponding authors.
E-mail addresses: chen@szu.edu.cn (Z. Chen), cslao@szu.edu.cn (C. Lao).

https://doi.org/10.1016/j.jeurceramsoc.2018.11.013
Received 3 October 2018; Received in revised form 30 October 2018; Accepted 5 November 2018
0955-2219/ © 2018 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/BY/4.0/).

Please cite this article as: Chen, Z., Journal of the European Ceramic Society, https://doi.org/10.1016/j.jeurceramsoc.2018.11.013
Z. Chen et al.
Table 1
Ceramic 3D printing technologies.
Feedstock form Ceramic 3D printing technology type Abbreviation
Slurry-based Stereolithography SL
Digital light processing DLP
Two-photon polymerisation TPP
Inkjet printing IJP
Direct ink writing DIW
Powder-based Three-dimensional printing 3DP
Selective laser sintering SLS
Selective laser melting SLM
Bulk solid-based Laminated object manufacturing LOM
Fused deposition modelling FDM
above-listed 3D printing technologies used for the manufacturing of
ceramic components. Overviews of each technology will be given, with
representative examples of as-prepared parts presented. The historical
origins and evolution of each type of technology will be specifically
emphasised. Moreover, a thorough comparison of important aspects of
the ceramic 3D printing technologies will be presented.
2. Slurry-based technologies
Slurry-based ceramic 3D printing technologies generally involve
liquid or semi-liquid systems dispersed with fine ceramic particles as
feedstock, either in the form of inks or pastes, depending on the solid
loading and viscosity of the system. The slurry content can be 3D
printed by either photopolymerisation, inkjet printing or extrusion.
Advances in materials science have also made it possible to photo-
polymerise pre-ceramic polymers (PCPs) for transformation into
polymer-derived ceramic (PDC) components via heat treatment. In this
section, photopolymerisation-based techniques such as stereo-
lithography (SL) and its derivatives, i.e. digital light processing (DLP)
and two-photon polymerisation (TPP), along with inkjet-based inkjet
printing (IJP) and extrusion-based direct ink writing (DIW) will be
discussed.
2.1. Stereolithography (SL)
The SL technique is believed to be the most prominent and popular
3D printing technology and has been extensively used worldwide [5]. It
was first proposed and developed by Hull in 1986 [6] and was later
commercialised by 3D Systems Inc. SL is a process in which a light
source of a certain wavelength (usually in the ultraviolet range) is used
to selectively cure a liquid surface in a vat containing mainly photo-
polymerisable monomer along with other additives in very small
amounts, particularly photoinitiators [7]. The light-activated poly-
merisation process (i.e. liquid monomer turns into solid resin) generally
proceeds point-to-line, line-to-layer, then layer-by-layer, along with the
light scans on the liquid surface. When polymerisation is finished for
one layer, the vat or platform supporting the part being produced is
lifted or lowered by the thickness of a layer, depending on whether the
building process is being operated in a top-down or bottom-up mode.
Sometimes, a wiper blade is required to level off the liquid surface
before the next layer is printed. SL is capable of fabricating parts of high
surface quality at fine resolutions down to the micrometre scale. A
schematic diagram of a typical SL technique is shown in Fig. 1. To aid
visualisation, it should be noted that the feedstock materials shown in
the schematic diagrams in this review are rendered with translucent
colouring.
The SL of ceramics proceeds with the addition of fine ceramic par-
ticles, down to micro/nanometre size, into the photocurable medium,
which can be aqueous or non-aqueous [8,9]. The liquid becomes a
ceramic suspension after it has been well dispersed in the medium with
the aid of essential surfactants and additives. Similarly, polymerisation
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Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
Fig. 1. Schematic diagram of the stereolithography (SL) process.
only takes effect in the organic monomer phase under light irradiation
as ceramic particles are inert to light emission. The ceramic particles
are then uniformly surrounded by the cross-linked organic network
being polymerised to form the pre-designed shape of each layer until
the entire 3D ceramic part is built up. The green parts have to be
processed with further treatments, typically pyrolysis to remove or-
ganics followed by sintering at high temperatures to reach the packed
density, much the same as in conventional ceramic processing routes
such as injection moulding [10]. There is also an indirect SL method, in
which SL resin moulds are prepared for investment casting of complex
ceramic parts [11]. In this review, only direct SL is discussed.
The SL process has been pioneered and extensively studied by
Halloran and co-workers [8,12–15] since 1994, starting with the use of
highly concentrated ceramic suspensions up to 65 vol%, including si-
lica, alumina and silicon nitride. To successfully carry out the process, a
number of requirements must be fulfilled. Of primary importance to the
process are the ceramic suspensions. They should possess appropriate
rheological behaviour, including long-term stability and suitable visc-
osity. The ceramic particles must be homogeneously and effectively
dispersed in the photopolymerisable medium and remain stable without
severe particle segregation for a reasonable period of time (e.g. hours to
days). Unstable suspensions with rapid segregation could lead to ma-
terial inhomogeneity in the fabricated parts. A good candidate for a
ceramic suspension should also retain a satisfactory viscosity for proper
flow during the printing process. At the beginning of ceramic SL de-
velopment, suspension viscosity had to be comparable with that of
commercial resin (less than 3000 mPa·s) [8], whereas current SL is also
capable of working on suspensions of tens of Pa·s at a shear rate of 1000
s−1. However, this is often challenging because, on the one hand, a
higher volume fraction of ceramic particles is favourable for less
shrinkage and greater density (and thus mechanical strength) after
sintering, while, on the other hand, a lower ceramic loading is usually
required to minimise the viscosity and avoid possible segregation of the
solid content. Therefore, compromises have to be made to prepare
suitable ceramic suspensions for SL.
Another fundamental problem that has to be considered is the non-
trivial effect of light scattering arising directly from the ceramic parti-
cles added into the suspensions, even when the particles themselves are
transparent to irradiation. Such scattering is unfavourable to light pe-
netrating into the suspension, but at the same time undesirably
broadens the lateral curing area (i.e. curing width), which greatly af-
fects the overlap behaviour of the curing units and thus the dimensional
accuracy of SL [16]. The curing depth (and thus the layer thickness) is
then associated with the ceramic particle size and volume fraction, light
exposure power, and the reflective index of the materials [8,17]. Of
particular importance is the difference in refractive index between the
photopolymerisable medium and the ceramic particles. Ceramic parti-
cles exhibiting greater light absorption and refraction under exposure to
the photopolymerisation wavelength can be highly challenging to
process [18].
Badev et al. [19] studied the polymerisation kinetics of a series of
Z. Chen et al.
Fig. 2. (a) Influence of the refractive index (SiO2 < Al2O3 < ZrO2 < SiC) and (b) ceramic particle concentrations and alumina particle size and solid loading on the
photopolymerisation conversion of a ceramic filler containing acrylate [19].
suspensions filled with different ceramic particles (i.e. SiO2, Al2O3,
ZrO2 and SiC). They found that the refractive index ratio between the
ceramic particles and the organic content, as well as the viscosity, were
the main parameters governing the reaction and hence the final poly-
merisation rate (i.e. conversion) in the suspensions. The polymerisation
rate decreases with increasing index ratio as a result of light scattering
and absorption, which is worse for larger particle sizes, as shown in
Fig. 2. This causes the SL of SiO2 [20] and Al2O3 [21] to be easier than
that of ZrO2 [22] and SiC [18]. Therefore, smaller ceramic particles
with better light-scattering properties are preferred in SL.
Ceramic SL has been extensively developed and applied to the
fabrication of dense/cellular ceramic parts in a number of fields, ran-
ging from parts with complex structures such as integrally cored casting
moulds [23–25], microelectronic components such as sensors [26,27]
and photonic crystals [28,29], to biomedical implants such as bone
scaffolds [30,31] and dental components [32,33]. Progress has also
been made on some other concerns in ceramic SL arising from the ef-
fects of residual monomer content [34], ceramic particle segregation
[15], light curing strategy [35] and the debinding process [36]. Fig. 3
demonstrates some advanced ceramic parts fabricated using SL.
Most suspensions used in SL are non-aqueous and are based on ac-
rylamide or resin because aqueous-based suspensions would result in
lower green strength. Chen et al. [9] used an improved aqueous-based
suspension in which silica sol was used instead of deionised water to
maintain good green-part strength and lower viscosity.
More recently, instead of suspensions that are homogeneously dis-
persed with the fine ceramic particles used in SL, PCPs in liquid form,
such as silicon oxycarbide, have been increasingly used for photo-
polymerisation [37,38]. The solid parts of PDCs can be obtained by
sintering and ceramisation of the polymerised parts at high
Fig. 3. Advanced ceramic parts fabricated using SiO2 via SL [9]: (a) porous bioceramic scaffold; (b) photonic crystals; (c) hollow turbine blade; (d) impeller; (e)–(f):
investment casting moulds.
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temperatures. This makes the process a viable alternative to ceramic SL.
PDCs are high performance and possess versatile and advantageous
functionalities that can be adjusted by varying the compositions and
structures of the PCPs [37,39–41], such as introducing multiple metal
alkoxides [42]. A number of demonstrations have been made of the use
of SL on PCPs to produce PDCs with complex and delicate structures,
including SiC [18] (Fig. 4) and SiOC [43].
2.2. Digital light processing (DLP)
The digital light processing or digital light projection (DLP) tech-
nique is in fact a mask-based SL, in which an integral image is trans-
ferred to the photopolymerisable liquid surface by exposing the light
source through a patterned mask once only. The original concept was
first proposed by Nakamoto and Yamaguchi in 1996 [44] using physical
masks. It was further developed and improved on by Bertsch et al. in
1997 [45] with the use of a liquid crystal display (LCD) as the dynamic
mask generator. Since 2001, progress has been made by replacing LCDs
with digital micromirror devices (DMDs) from Texas Instruments owing
to their competitive fill factor and reflectivity (resulting in higher re-
solution and contrast in the light display) [46–48]. A DMD is a chip that
consists of a rectangular array of several hundred thousand microscopic
mirrors corresponding to the pixels in the image to be displayed. Ac-
tuated by electrostatic forces, the micromirrors function as ultra-fast
light switches and can be individually rotated by ± 10–12° to an ‘on’ or
‘off’ state. The incident light beams with a spatial resolution of 1.1 μm
are accordingly reflected to pass through/deviate from the lens, making
the pixels appear bright/dark on the projection surface (i.e. screen)
[49]. Details regarding the functioning mechanism of DMDs can be
found elsewhere [50,51]. The ultra-fast light switching and integral
Z. Chen et al.
Fig. 4. SiC parts prepared by SL on pre-ceramic polymers. Comparison of printed and sintered samples (bottom) [18].
Fig. 5. Schematic diagram of the DLP process.
projection allow the DLP 3D printing process time to be dramatically
reduced as it is much faster than the conventional SL point-line-layer
scanning process. Moreover, very good feature resolution can be ob-
tained, to several micrometres. These remarkable advantages of DLP
technology have attracted considerable attention in the 3D printing
industries, and it has been explored for fabricating parts with even
higher accuracy and speed [52–56]. The DLP technique is also referred
to as projection micro-stereolithography, or PμSL. Fig. 5 shows a
schematic diagram of the DLP process. In this figure, the exposure of the
individual layers takes place from below through the transparent ma-
terial vat.
The use of the DLP technique as a 3D printing tool in ceramics
fabrication has been widely explored. High-density (97–99%) zirconia
and alumina structural parts with a Vickers hardness (13.1 and
17.5 GPa, respectively) comparable with those prepared using con-
ventional approaches have been produced [57,58]. Since 2012, con-
siderable efforts have been made by a research team at Vienna Uni-
versity of Technology using DLP for the production of complex ceramic
structures with very fine features based on materials including alumina
and bioactive glass, with resulting relative densities above 90% and
mechanical strength comparable with conventionally processed sam-
ples [59–62]. The feature resolution generated reached 25 × 25 × 25
μm3. Fig. 6 shows the fabricated samples. Other ceramic materials such
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Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
as zirconia and β-tricalcium phosphate (β-TCP) were also successfully
printed with solid loadings of up to 50 vol% [63].
It is worth noting that, based on the above work, the team com-
mercialised the DLP ceramic printing technique, which they called li-
thography-based ceramic manufacturing (LCM), by founding Lithoz
GmbH for further development of the 3D printing of advanced fine
ceramics [64]. A substantial amount of work has been performed using
LCM machines, particularly for the preparation of cellular ceramic
structures with very small feature sizes, such as honeycomb catalyst
supports [65], heat exchangers [66] and negative Poisson’s ratio me-
tamaterial structures [67]. Examples are shown in Fig. 7.
In addition, the DLP technique has been used to print PDC structures
with high resolution. This was successfully demonstrated by Zanchetta
et al. [43] who prepared complex dense and crack-free silicon oxycar-
bide 3D structures with micrometre-scale features. The higher effi-
ciency of DLP over the conventional SL process makes it a promising 3D
printing technique for ceramics fabrication.
2.3. Two-photon polymerisation (TPP)
In recent years, there has been an increasing demand for nanoscale
fabrication of 3D microstructures, particularly in the fields of nano-
biomedicine, nanoelectronics and nanomechanics. Growing advances in
materials chemistry and laser optics have made it possible to develop
novel nanofabrication techniques. Among them is two-photon poly-
merisation (TPP), in which the polymerisation is activated by the si-
multaneous absorption of two photons (TPA) of a near-infrared
(780 nm) or green (515 nm) laser, only taking place at high laser in-
tensity within a spatially localised focal spot in the corresponding
photosensitive resin [68]. A schematic diagram of the process is shown
in Fig. 8.
The advantage of TPP as a micro/nanofabrication tool lies in its
ability to polymerise submicron focal volumes inside the polymer li-
quids through TPA. This is not possible with conventional one-photon-
based processes (such as SL), in which polymerisation takes place only
on the liquid surface [69]. A TPP resolution that is confined to less than
200 nm or close to the diffraction limit can be achieved owing to the
Z. Chen et al. Journal of the European Ceramic Society xxx (xxxx) xxx–xxx

Fig. 6. Samples made with (a)–(b) alumina and

(c)–(d) bioglass using the DLP technique
[59,62].

quadratic dependence of the TPA rate on the incident intensity [70].

Experiments were undertaken by Wu et al. in 1992 [71] to verify the
possibility of 3D patterning, with the production of high-aspect-ratio
trenches of simple shapes. The feasibility of TPP in the fabrication of
complex 3D microstructures was then demonstrated by Maruo et al. in
1997 [72], with the preparation of spiral structures of 7 μm diameter
using a urethane acrylate resin. Following this, the technique has been
extensively explored by a number of research groups across the world in Fig. 8. Schematic diagram of the TPP process, with inset showing that the focus
the fields of photonic components and micromachines [73–80]. Fea- of the laser beam drives the polymerisation process.
tures with lateral resolutions below 100 nm have previously been de-
monstrated. Fig. 9 demonstrates examples of polymer-based 3D pho-
flexible design of structure porosity and pore dimensions [85].
tonic crystals fabricated using TPP with very complex microstructures
There has been an increasing demand for nanoscale fabrication of
and fine features [81].
high-quality ceramic nanostructures. Progress has been made on ex-
While the above developments have all been made using polymeric
ploring the fabrication of hollow-tube ceramic nanolattices based on
materials, the need for resistance to harsh environments has given rise
the processing route associated with TPP, which proceeds as follows. A
to the demand for ceramic components with complex 3D micro-
3D polymer structure with a feature size down to the nanometre scale is
structures and nanoscale feature sizes to be manufactured using nano-
first created by TPP, followed by infiltration of ceramic nanoparticles
fabrication processes. The unique capacity of TPP for submicron re-
using chemical vapour deposition (CVD) or atomic layer deposition
solution processing has paved the way to achieving this. To this end,
(ALD), after which the structure is milled on one surface using a fo-
Pham et al. [82] reported the first use of TPP for fabricating real 3D
cused-ion beam (FIB) or reactive-ion etching (RIE) to uncover the em-
SiCN woodpile nano/microceramic microstructures of submicron re-
bedded polymer, allowing openings for the removal of the polymer by
solution. The study was undertaken based on a synthesised inorganic
chemical etching or oxygen plasma etching, leaving behind a hollow
pre-ceramic polymer photoresist with high photosensitivity and a high
truss structure [86,87]. In this way, SiO2 [87], TiN [88] and Al2O3 [89]
ceramic yield. Preliminary results showed a linear shrinkage of up to
hollow-tube nanolattices with superior optical or mechanical properties
41% after pyrolysis, which was then rectified by introducing 10 nm
were successfully fabricated. Fig. 11 shows the design and the fabri-
silica particles at a solid loading of 40 wt%. Fig. 10(a)–(h) demonstrates
cated TiN ceramic hollow-tube nanolattice [88].
the fabricated SiCN samples. Following this, they later reported [83]
The above studies show TPP’s unique ability to process highly
the fabrication of SiC ceramic microstructures with near-zero shrinkage
complex ceramic parts and achieve extremely high accuracies of sub-
after pyrolysis based on a new photosensitive precursor system using a
micron resolution. However, TPP’s working principle of cross-linking
bifunctional inorganic polymer. More recently, Colombo et al. [84]
materials at subsurface locations of the feedstock liquid limits it to
reported the fabrication by TPP of a complex, highly porous SiOC
using only polymeric materials (including the pre-ceramic polymers)
diamond structure at the micron scale based on a pre-ceramic polymer
that are ‘transparent’ and thus accessible to the incident laser. As a
(Fig. 10(i)). TPP was also used for the fabrication of 3D Zr–Si polymer
consequence, the ‘opaque’ ceramic slurries that are commonly used in
ceramic scaffolds for autologous bone tissue engineering, allowing the
SL and DLP processes cannot be worked with TPP. Moreover, TPP

Fig. 7. Sintered alumina parts fabricated using the LCM technique: (a) gear wheels; (b) turbine blade; (c) cellular cube [63]; (d) auxetic structure with micrometric
details; (e) detailed features of the unit cell [67]; (f) pipe-shaped heat exchanger with complex 3D structures [66].

5
Z. Chen et al.
Fig. 9. Scanning electron microscopy (SEM) images of different complex spiral-shaped microstructures fabricated using the TPP technique: (a) integral U-shaped
spiral block; (b) individual U-shaped spirals; (c) U-shaped spiral block with L-shaped waveguides; (d) circular spiral block [81].
produces only parts of very small sizes at the micro scale, and longer
production times are generally needed owing to the extra-fine preci-
sion.
2.4. Inkjet printing (IJP)
IJP is a well-known method for creating two-dimensional digital
text and images by means of ejecting liquid-phase materials (i.e. ink) in
droplet form through printhead nozzles onto paper, plastic or other
substrates [90]. The technique is widely used nowadays, with various
types of printers on the market ranging from compact and cheap con-
sumer models to large and expensive industrial machines. IJP tech-
nology was first developed in the 1950s, and the commercialisation of
computer-aided IJP took place only after the 1970s, mainly by com-
panies such as Epson, HP and Canon [91]. IJP can be operated in one of
two modes: continuous or drop-on-demand (DOD) [92]. DOD mode is
preferred in 3D printing owing to its higher positioning accuracy and
smaller droplet size and can be realised by squeezing ink through either
thermal excitation or the piezoelectric effect. IJP has since been further
developed as a material deposition technique for thin-layer deposition
onto substrates. The range of ink materials has been extended, to in-
clude polymers or metals for electronic patterning [93,94], solder paste
for microelectronics soldering [95] and cells for restoration in tissue
engineering [96], where the printed components might occur in 2D
structures and would not necessarily possess proper 3D features.
Nevertheless, IJP is limited to printing miniaturised parts owing to the
very small volume of the feedstock material (i.e. ink) used, as currently,
commercial printers eject only a few picolitres to nanolitres of ink per
single droplet.
In recent years, much progress has been made on transforming the
technique into a versatile manufacturing process for 3D fabrication of
multilayered parts. There has been a growing interest in the IJP of
ceramic inks where ceramic particles are well dispersed within a liquid
solvent for direct and selective deposition onto a substrate through a
printhead. Computer-aided high-precision positioning of the droplet
jetting allows a point-line-layer-part building process. A solid ceramic
phase can be created after proper drying and sintering of the printed
materials. A schematic diagram of IJP for ceramics printing is presented
in Fig. 12.
The application of IJP to printing ceramic components was first
described in the literature by Blazdell and co-workers beginning in
bottom and top. These were fabricated using a resin containing 40% silica particles (each inset is the top-view of the structure) [82]; (i) unpyrolysed SiOC diamond
structure fabricated using the TPP technique [84].
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Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
1995 [97,98] using ZrO2 and TiO2 ceramic inks, both of volume frac-
tions as small as 5 vol%. Such low volume fractions would lead to long
drying times. However, their earlier attempts at ceramic printing gen-
erated only simple multilayer structures, as shown in Fig. 13(a)–(c),
which also exhibited poor surface quality. The group then successfully
printed small-sized pillar arrays based on submicron ZrO2 particles
loaded at 14 vol% in the ink [99], as shown in Fig. 13(d). The pro-
nounced influence of different ink properties, in particular the viscosity
and surface tension, on the printing behaviour was studied. Seerden
et al. [100] later reported the use of ceramic ink prepared with an Al2O3
loading of up to 40 vol%, resulting in the fabrication of ceramic parts
with a feature size of less than 100 μm. Fig. 13(e)–(f) shows images of
the as-prepared unfired structures.
The performance of IJP of ceramics very much hinges on the critical
factors of the ceramic powder and ink formulation as well as their
properties, in particular the rheological characteristics such as dis-
persivity, stability, viscosity and surface tension. In addition, a mod-
erate pH value must be maintained to prevent possible corrosion of the
jetting system by the ink. A uniform particle size distribution with
particles less than 1/100 of the nozzle diameter (at the micron scale)
can prevent the clogging and blockage of nozzles and capillaries, as
required by the printer manufacturers [94]. Thus, adequate filtering is
generally applied to remove larger particles. In general, nanoparticles
are more desirable in formulating inks. However, smaller particles are
more likely to undergo agglomeration within the inks. Therefore,
homogeneous dispersion of the ceramic powder within the ink is a
crucial prerequisite for the ink to pass smoothly through the printhead
nozzles. The ejection behaviours of ceramic inks are largely determined
by their viscosity. Insufficient jetting or too high a velocity may result
from too large or too small a viscosity, respectively [101]. Ceramic inks
often possess low viscosities, down to a few mPa·s, as a result of low
solid loading, causing a lengthy drying time and considerable
shrinkage, which could adversely affect the final accuracy of the printed
part. An increase in solid loading might be beneficial, but this can lead
to changes in the ink’s rheological behaviour. Therefore, various opti-
misations and compromises need to be made to ensure that proper solid
loading and rheological properties are achieved. Seerden and co-
workers [102,103] showed that the use of alumina wax ink could
minimise drying shrinkage, while good sintering density remained
difficult to achieve. More recently, Chen et al. [104] have reported a
detailed investigation of the optimisation of different formulations,
Fig. 10. SiCN woodpile structure fabricated
using the TPP technique: (a) design of the
structure; (b) polymeric structure with no filler;
(c) ceramic woodpile structure without filler;
(d)–(f) ceramic woodpile structure obtained
from the mixed resin containing various
amounts of silica filler for reduced shrinkage:
(d) 20 wt% silica, (e) 30 wt% and (f) 40 wt%.
Other 3D ceramic microstructures of spiral
shape: (g) micro-tube and (h) micro-cruciform
with a twisting angle of 90° between the
Z. Chen et al.
Fig. 11. (a) CAD design of an elliptical hollow-tube nanolattice, with the enlarged part being an octahedron unit cell; (b) SEM image of the FIB-milled edge of a
nanolattice. The top left inset shows a transmission electron microscope (TEM) image of the microstructure, revealing nano-size grains. The bottom left inset shows a
zoomed image of the hollow tubes; (c) SEM image of the full structure. The scale at the bottom shows a comparison of the approximate sizes of the components of the
structure [88].
Fig. 12. Schematic diagram of the IJP process, with inset showing the print-
head jetting droplets at a higher magnification.
particularly with regard to the dispersivity and other rheological
properties of an aqua-based ceramic ink used for printing solid oxide
fuel cell cathode layers. Their results showed that a long-term stable
and printable ink with a well-dispersed ceramic powder was obtained
by tuning the ink’s zeta potential with the help of the interparticle
Derjaguin–Landau–Verwey–Overbeek (DLVO) theory [105].
A quality ink that is compatible with a DOD inkjet printer should
exhibit proper printing performance, which can then be described as
the ‘printability’ of the ink. A quantitative characterisation based on the
ink’s physical properties of such a printability was developed by Fromm
and co-workers [106], who proposed a ratio Z that is independent of the
ejection velocity and is the reciprocal of a dimensionless number – the
Ohnesorge number Oh – given by the formula:
1
Z = 1/Oh =
Re
=
( a) 2
We
where Re and We are the Reynolds number and the Weber number,
respectively. These numbers are expressed as Re = νρa/η and We =
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
ν2ρa/γ [107], where a is a characteristic length representing the radius
of the nozzle and ν, ρ, η and γ are the ejection velocity, density, viscosity
and surface tension determined for the ink, respectively. Research
[108] has suggested that for a printable ceramic ink its Z value should
fall within the range of 1–10. The ejection of droplets may be prevented
by viscous dissipation when Z is less than 1, and unwanted tiles or
satellite droplets can be formed when Z is greater than 10. This
guideline has also been widely applied in the IJP of ceramic inks
[109–113].
Another major concern in ceramic IJP is the coffee stain effect that
can occur in the course of drying of as-printed patterns [114]. Such an
effect manifests as the segregation of solid particles from the centre to
the edge of the printed patterns on the substrate, caused by convective
macroscopic flow into the contact line [115]. This problem can lead to
defects in the printed structure, and is mostly observed for inks with
low solid volume fractions. Measures have been taken to minimise such
effects. Dou et al. [116] prepared a 10 vol% ZrO2 aqueous ink dis-
playing a severe coffee stain effect during drying. The addition of 10 wt
% polyethylene glycol (PEG) to the ink helped to prevent the effect, but
it persisted when multilayer printing was attempted. By drastic short-
ening of the drying time with the addition of a fast drying agent (e.g.
50 vol% isopropyl alcohol), Friederich et al. [117] reported the re-
sulting rapid increase in viscosity after deposition and the complete
suppression of the coffee stain effect in a 10 vol% barium strontium
titanate (Ba0.6Sr0.4TiO3) ceramic ink.
In terms of further applications of IJP of 3D ceramic parts, growing
interest has been shown in the manufacture of functional components
used in microelectronics. IJP has been used to produce millimetre-scale
dense 3 mol% yttria-stabilised tetragonal zirconia (3Y-TZP) samples
(1) using a 24 vol% ink with a layer thickness of 300 μm for use in printed
circuit boards [118]. Bhatti and co-workers [119] printed lead zirco-
nate titanate (PZT, 2.5 vol% ink) micro-pillar arrays, which could be
Fig. 13. (a) Printed TiO2 multilayer coupons
before sintering; (b) after sintering [97]; (c)
printed 10 layers of ZrO2 on nitrocellulose
membranes [98]; (d) sintered ZrO2 fibre arrays
with 4900 layers [99]; (e) examples of un-
sintered ceramic bodies printed from 30 vol%
Al2O3 slurries; (f) enlarged image showing the
detailed feature printed [100].
7
Z. Chen et al.
Fig. 14. Micro-arrays of pillars: (a) PZT pillars of 1000 layers before sintering; (b) 4000 layers of printing [119]; (c) TiO2 pillars after sintering; (d) highly magnified
image of one pillar [120].
used as transducers for applications in medical imaging and non-de-
structive evaluation. Up to 4000 layers a few hundreds of microns tall,
equivalent to an average thickness of 0.4 μm, were obtained, as shown
in Fig. 14(a)–(b). More recently, Lejeune et al. [120] have also printed
PZT and TiO2 micro-pillar arrays with more detailed structures.
Fig. 14(c)–(d) shows the sintered samples printed using 15 vol% TiO2
ink.
Dense structural ceramic parts have been successfully fabricated by
Cappi et al. [121] using an aqueous Si3N4 ink with a 30 vol% solid
loading (Fig. 15). Mechanical properties comparable with those of dry-
pressed ones were achieved, suggesting the potential for IJP to fabricate
high-performance non-oxide engineering ceramics. Research [122] has
also reported that pre-ceramic polymers loaded with 10 vol% SiC par-
ticles and 7 vol% polycarbosilane generated low-viscosity inks suitable
for IJP. Their results showed that 3D parts can be fabricated with low
shrinkage and that no macro defects were detected.
Recently, special attention has been paid to the IJP of thin func-
tional layers used as electrodes in energy devices, such as solid oxide
fuel cells, based on non-oxide composite ceramic materials [123–127].
Most studies have focused on ink preparation and layer characterisa-
tion, while some have obtained electrochemical results comparable
with those fabricated using conventional deposition techniques [128].
Fig. 16 shows an SEM image of composite cathode layers printed with
LSM-YSZ [128] and LSCF-CGO [124].
Overall, IJP is a versatile 3D printing technique for printing small-
sized ceramic parts, albeit with limited flexibility in complex structure
design, such as the inability to print overhanging or hollow structures
due to difficulties with support preparation. However, the advantages
of low cost, a simple processing route and variety in the selection of
materials have greatly promoted its application in advanced ceramic
manufacturing, particularly in the microelectronics and energy device
domains.
2.5. Direct ink writing (DIW)
DIW, also known as robocasting (RC) [129], was first filed as a
patent by Cesarano and co-workers at Sandia National Laboratories in
1997 [130]. The technique was originally developed for processing
concentrated materials such as ceramic slurries with little organic
Fig. 15. Si3N4 gearwheel fabricated by IJP: (a) green part; (b) sintered part [121].
8
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
content. In fact, some [131] regard DIW as a broad description of an
assembly of 3D printing technologies that use ink (be it droplet or
paste) deposition to create designed structures. In this review, to have a
detailed understanding of the technique, the description of DIW is
centred on the extrusion method using a filament of a highly viscous
paste (analogous to conventional inkjet printing ink) at room tem-
perature, thus sticking to its original concept. The deposition manifests
itself as extrusion of the materials through nozzles whose openings are
required to be much larger than those of IJP nozzles owing to the higher
viscosity of the materials used. Objects are built up by moving nozzles
to directly ‘write’ the designed shape layer by layer until the part is
complete. Debinding and sintering then follow so that the part is free of
organics. A schematic diagram of DIW is shown in Fig. 17.
DIW enables a cheaper and faster manufacturing process compared
with photocuring 3D printing techniques. The use of semi-liquid pastes
allows for shape retention owing to the high solid loading and viscoe-
lastic properties. Therefore, DIW is able to fabricate freestanding
structures with high-aspect-ratio walls or spanning parts without the
need for supports (such as powder bed, liquid vat or printed supports),
which is not possible with other 3D printing techniques [132]. A great
range of different structures can be created using this technique, from
solid monolithic parts [133] to complex porous scaffolds [131] and
composite materials [134]. Small-sized electronic components as well
as woodpile lattice structures have shown considerable prospects in the
domains of piezoelectric components such as transducers [135–137],
bandgap structures such as photonic crystals [138–140], catalyst car-
riers that can be used in energy devices [141,142], filters [143,144],
and tissue engineering [145–147].
Smay and co-workers [148,149] from Harvard University have
made great progress in the DIW of 3D periodic structures, with char-
acteristic feature sizes ranging from micrometre to millimetre scales.
Fig. 18 depicts representative images of such 3D structures produced
using gel-based 47 vol% PZT paste [150]. The structures serve as the
active element in 3-3 piezoelectric–polymer composites. This example
shows the great potential of continuous DIW for fabricating complex 3D
structures.
Sun and co-workers [141] have pioneered opportunities for using
DIW to prepare electrodes for lithium-ion (Li-ion) batteries. High areal
energy and power densities were achieved with printed high-aspect-
Z. Chen et al.
Fig. 16. (a) SEM image of the cross section of printed LSM and LSM-YSZ layers [128]; (b) LSCF-CGO printed cathode layer [124].
Fig. 17. Schematic diagram of the DIW process, with inset showing the nozzle
extruding ceramic feedstock.
ratio cathode and anode structures. More recently, Liu et al. [142] re-
ported the use of low-temperature DIW for the preparation of LiFePO4
electrodes. Their results showed improvements in the performance of
printed electrodes due to their highly porous structures as a result of
low-temperature printing.
It is worth noting that, to date, the fabrication of bioceramic im-
plants is one of the most studied applications [151–153]. The porous
lattice structures within the fabricated implants are beneficial for the
growth of human body tissues for transplant. In addition, advances in
medical imaging technology now allow real microstructural models of
the part to be repaired to be reproduced in accurate 3D digital format.
This can further aid the 3D printing of the artificial part with precise
geometries very similar to the original missing part. The excellent
biocompatibility and the porous structural similarity to bone of calcium
phosphate glasses and hydroxyapatite (HA) have considerably boosted
research into the fabrication of artificial bone scaffolds [154–156].
Fig. 18. (a) 3D periodic PZT structures made by DIW with concentrated ceramic paste; (b) SEM image showing the detailed microstructure [150].
9
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
Simon et al. [146] reported excellent results for bone growth using
HA scaffolds fabricated by DIW with 3D periodic pore architectures
(Fig. 19). The ability to build multiscale porosity mimicking the natural
microstructure of human bone shows great promise for bone repair and
replacement.
A customised load-bearing mandible bone implant with a lattice
structure was successfully fabricated by Cesarano et al. [157] using
DIW of HA paste, based on 3D computed tomography (CT) scan-aided
modelling. Submicron pores were created with controlled sintering, and
good mechanical performance was achieved. The implant surgery and
subsequent testing showed a good fit with the defect region of the pa-
tient. Such customised implants may replace tedious autograft pro-
cesses, thereby eliminating bone harvesting operations, which would
effectively reduce the cost, time and complexity of the surgery. Fig. 20
shows the CT-aided design of the bone, the printed bone implant pos-
sessing various levels of porosities and the fitting of the implant to the
patient’s defect region.
In a study carried out by Cesarano et al. [129], filament formation
and initial shape retention were achieved by adjusting the paste visc-
osity, yield strength and drying kinetics. Shrinkage and cracks caused
by drying were minimised by increasing the solid volume fraction up to
64%. Advanced metal matrix and ceramic matrix composites that can
withstand harsh environments such as ultra-high temperatures can be
formed by infiltrating woodpile bodies with molten glasses, alloys or
slurries. A metal–ceramic composite part with a 3D periodic structure
was successfully created by pressure infiltration with liquid aluminium
of an alumina tower fabricated by robocasting of Al2O3–ZrO2 gel paste
[136] (Fig. 21). Promising results, including a very low thermal ex-
pansion coefficient and compressive strength much greater than that of
the uninfiltrated ceramic preform, were obtained with little increase in
density after infiltration. Filaments with various cross-sectional
Z. Chen et al.
Fig. 19. Optical micrographs of hydroxyapatite (HA) scaffolds prepared by DIW, with four distinct periodic arrays [146].
features, such as square, hexagonal and even hollow micron-sized
shapes, can be prepared with the corresponding micro-machined nozzle
tips [158,159].
In terms of structural engineering ceramics fabrication, very re-
cently, Eqtesadi et al. [160] reported for the first time the use of DIW
combined with pressureless spark plasma sintering to fabricate geo-
metrically complex B4C components. Adequate mechanical properties
were obtained, with sintered densities of up to 90%. The printed
structures are shown in Fig. 22.
In addition, other variants of DIW have been developed for high-
quality ceramic printing, among which is freeze-form extrusion fabri-
cation (FEF) proposed by Leu and co-workers [161]. The main differ-
ence between FEF and the fused deposition of ceramics (FDC) lies in the
building environment, which is below the freezing point of water for
the solidification of the printed materials. Functional CaCO3 compo-
nents with graded colours (Fig. 23(a) and (b)) and multiple ceramic
parts with graded compositions between Al2O3 and ZrO2 (Fig. 23(c))
were successfully fabricated with the aid of three extruders mounted on
the FEF system [162].
PCPs also show their promising and distinct suitability to the ap-
plication of DIW. The rheological behaviour of the feedstock can be
optimised by the addition of PCPs, and fillers/dopants introduced into
PCPs at the same time can help to modify the composition/phase,
structures and properties of the final product after heat treatment [84].
Oxide powders or precursors such as carbonates or hydroxides mixed
with a silicone resin for DIW have been reported to generate single-
Fig. 20. (a) Designs of the mandible bone and the defect region (isolated view); (b) printed bone implant lattice at different view angles; (c) various levels of
porosities present in the sintered lattice; (d) fitting of the bone implant to the patient’s defect region [157].
10
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
phase [147] or multiphase [134] ceramic parts with adequate perfor-
mance suitable for tissue engineering applications. The desired SiO2
phase was also obtained after reactions with the oxide powders during
firing in air. Taking advantage of the unique formability of a PCP (e.g.
polymethylsilsesquioxane, PMS) acting as both polymeric binder and
SiOC ceramic source, Franchin et al. [163] reported the development of
an ink containing chopped microfibres suitable for DIW, enabling
ceramic matrix composite structures with complex shapes to be fabri-
cated. Their study [164] demonstrated that the addition of a small
amount of graphene oxide below 0.1 wt% helped to improve the
structural stability during firing and reduce the shrinkage of the PCP.
The fabricated SiOC composite components exhibited electrical con-
ductivity due to the loss of oxygen functional groups from the graphene
oxide fillers as a result of firing. One particularly favourable practice in
the fabrication of bioceramic scaffolds is the creation of secondary
porosity by the decomposition of fillers after firing, which is useful for
cell cultivation.
Thus, DIW is well suited to the fabrication of tailored porous
ceramic structures possessing periodic features, with little or no surface
quality/resolution needed. In this sense, dense engineering ceramics are
difficult to process using DIW, thus limiting its applications.
3. Powder-based technologies
Powder-based ceramic 3D printing technologies mainly utilise
powder beds normally containing loose ceramic particles as feedstock.
Z. Chen et al.
Fig. 21. (a) Side view of the tower structure; (b) idealised 3D design [136].
Fig. 22. Photos of dried structural B4C parts prepared using DIW [160].
The ceramic particles are bonded either by spreading liquid binders or
by powder fusion using thermal energy provided by a laser beam.
Therefore, in this section, three types of powder-based 3D printing
techniques are discussed, namely, three-dimensional printing (3DP),
selective laser sintering (SLS) and selective laser melting (SLM). The
former technique applies printheads to selectively jet liquid binder
droplets onto the powders, whereas the latter two use the energy of
Fig. 23. (a) and (b) Pink- and green-coloured CaCO3 parts fabricated using DIW with and without mixing; (c) test bar fabricated with 100% Al2O3 to 50% Al2O3 +
50% ZrO2 [162].
11
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
laser beams to selectively sinter/melt ceramic powders. Be aware of the
difference between the terms ‘3DP’ and ‘3D printing’. The abbreviation
‘3DP’ is retained for the individual 3D printing technique for historical
reasons, whereas ‘3D printing’ is now a general and popular term re-
presenting the assembly of additive manufacturing technologies.
3.1. Three-dimensional printing (3DP)
The 3DP method was first devised by Sachs et al. at the
Massachusetts Institute of Technology (MIT), who filed a patent for it in
1989 [165]. Although 3DP can be considered an indirect ceramic inkjet
printing process, its distinctive feature is the use of powder beds, which
is why 3DP is classified as a powder-based technique in this review. In
the process of 3DP, organic binder solution in droplet form is sprayed
through printheads onto selected regions of a powder bed surface. Solid
layers are formed by the solidification (i.e. gluing) of the permeating
liquid binder, which encloses the powder. A new layer of powder is
then supplied and spread on the previous layer to repeat the building
process until the part is formed. After this, loose powder is removed to
reveal the part. A schematic diagram of 3DP is depicted in Fig. 24.
The powder may be deposited in either a dry or a wet state in a
liquid vehicle (for a higher green density) [166,167]. However, the li-
quid content must be evaporated before the inkjet application of the
binder material. Desired characteristics, such as appropriate rheological
properties, have to be satisfied for the binder solution to be successfully
ejected through the printheads. Sintering is generally required to re-
move the organic binder so that the desired mechanical properties can
be obtained. Typically, this post-treatment process also causes
shrinkage of the part depending on the percentage of binder present.
The 3DP method was originally designed to rapidly produce com-
ponents from a larger variety of materials than was possible by the
Z. Chen et al. Journal of the European Ceramic Society xxx (xxxx) xxx–xxx

Fig. 24. Schematic diagram of the 3DP process, with inset showing the print-
head jetting binder solution.
other existing AM techniques available at that time, such as SL, SLS and
LOM [165]. The feedstock materials mentioned included ceramics
[168], metals [169] and plastics [170] in particle forms, as well as their
combinations [171]. Previously, an exclusive licence for ceramic 3DP
was held by the Soligen company [172]. Currently, however, machines
for the 3DP of ceramics are more popularly commercialised by com-
panies such as ExOne and 3D Systems [173].
The application of the 3DP method to ceramics fabrication was ori-
ginally reported in the 1990s with the use of alumina and silicon carbide
particles as powdered materials and colloidal silica as a binder [168].
One useful application is the fabrication of ceramic mould shells and
cores for metal casting [174]. The method was also used to fabricate
structural components with even larger sizes of up to several metres, as
reported by Cesaretti et al. [175]. More recently, the 3DP method has
been extended to other commercial applications owing to its consider-
able flexibility with respect to materials and geometries [176]. In par-
ticular, promising explorations have been made in the biomedical field,
including the fabrication of components for tissue engineering, which
generally require less precision in resolution and surface finish, as well as
porous features of the printed parts for cultivation purposes. Biocompa-
tible ceramics such as HA [177], calcium phosphates (CP) [178] and
tricalcium phosphate (TCP) [179] are often used in 3DP to print scaffolds
for bone replacement. Recently, Zocca et al. [180] used a pre-ceramic
polymer (silicon resin) as a binder, which also reacted with the fillers to
form desired ceramic phases, to print CaSiO3-based biocompatible
ceramic parts with a porosity of approximately 64 vol%. In vitro tests
indicated reasonable cell viability and no cytotoxic effects on the cells.
Fig. 25 shows examples of typical scaffolds printed using HA and CP,
showing features of coarse resolution [177,178].
To date, extensive studies have been conducted on a number of as-
pects, including ceramic powder and binder properties, binder–powder
bed interaction and process parameters. In a study focusing on the in-
vestigation of binder performance [181], Moon et al. found that the
molecular weight of the organic binder dominates the penetration
behaviour when spread onto a ceramic powder bed. It was suggested that
the molecular weight should be less than 15,000 for the binder to pe-
netrate. This study also reported that rheological properties such as the
surface tension and viscosity of the binder should be optimised to ap-
propriate levels for smooth jetting and high dimensional accuracy.
Lauder et al. [182] concluded that microstructures and surface finish
may be improved by optimising process parameters such as layer spa-
cing, line spacing and droplet spacing and placement. On the other hand,
a finer powder results in a smoother and thinner layer, but becomes more
difficult to spread over the working surface [183,184]. Studies have also
shown that lowering the layer thickness reduces the porosity effectively,
and thus improves the mechanical properties [185]. The resolution of the
printed parts also depends on the size and shape of the powdered ma-
terial as well as the features of the binder droplet. The interaction be-
tween the binder and the powder and the spreading speed of both
powder and binder also play important roles [186].
Porosities often remain larger for parts produced using 3DP com-
pared to other AM methods such as SLS and SLM [187]. Although
porosities seem advantageous in scaffold applications, they are un-
desirable in high-performance ceramics, which are mostly fully dense.
Difficulties in printing dense ceramics would limit the use of 3DP. Ef-
forts have therefore been made to minimise such a density limitation by
taking extra measures in post-processing [188], such as adding sin-
tering aids, infiltration of the porous parts and isostatic pressing prior to
sintering. Fielding et al. [189] reported a decrease in porosity from 9.2
to 6.9 vol% with the help of ZnO and SiO2 as sintering aids in the
printed TCP structures. Nan et al. [190] showed that liquid silicon in-
filtration at elevated temperatures reacted with TiC to yield Ti3SiC2-
based ceramics, resulting in an enhanced bending strength of 293 MPa
and a Vickers hardness of 7.2 GPa, while in an earlier study by Sun et al.
[191] on the preparation of Ti3SiC2 structures with complex geome-
tries, cold isostatic pressing was applied before sintering, after which a
very high density of 99% was finally obtained. The final parts are
shown in Fig. 26.
In general, the advantages of 3DP lie in the high flexibility of geo-
metrical design without the addition of supports. It is best suited to the
fabrication of porous ceramic parts. However, limitations of the appli-
cation of 3DP in the processing of advanced ceramic materials arise as
the downsides of this technique, in particular the inferior quality in
resolution, surface finish, density and mechanical performance, require
extra work, including infiltration and isostatic pressing for further
quality improvements.
3.2. Selective laser sintering (SLS)
SLS was invented by Deckard and Beaman at the University of Texas
at Austin, with the very first patent filed in 1986 [192], and was further
developed by the DTM company, which was acquired by 3D Systems in

Fig. 25. Scaffolds made by 3DP using biocompatible materials: (a) HA [177]; (b) CP [178], both showing features of coarse resolution.

12
Z. Chen et al.
Fig. 26. Final Ti3SiC2 structural parts obtained after cold isostatic pressing and
sintering [191].
Fig. 27. Schematic diagram of the SLS process.
2001. In an SLS process, as its name implies, a high-power laser beam is
used to selectively irradiate the surface of the target powder bed. The
powder then heats up and sintering (i.e. interparticle fusion) takes place
for bulk joining. After this, a new layer of powder is spread onto the
previous surface for the next run of heating and joining. In this way, the
process is repeated layer by layer until the designed 3D part is fabri-
cated. No extra support structures have to be intentionally prepared for
overhanging regions during an SLS process, as they are surrounded by
the loose powder in the bed at all times. A schematic diagram of the SLS
process is shown in Fig. 27.
The original intention of SLS was to make wax models for invest-
ment casting of metallic prototypes (e.g. aluminium). SLS has been
extensively studied to process a broad range of powdered materials,
starting with plastic and polymer powders of lower melting/softening
points [193–196], such as acrylonitrile butadiene styrene (ABS), poly-
vinyl chloride (PVC), polyether ether ketone (PEEK), polycarbonate
(PC), polyamide (PA) and other composites, and later extended to
metals (e.g. aluminium, iron and copper) and composite powders with
relatively higher melting points [197–199].
The feasibility of fabricating complex 3D ceramic parts using SLS was
first reported by Lakshminarayan and co-workers at the University of
Texas at Austin in 1990 [200,201] using Al2O3-based mixed powder
systems. As alumina has a melting point of as high as 2045 °C, secondary
components of ammonium phosphate (NH4H2PO4) and boron oxide
(B2O3) with lower melting points (190 °C and 460 °C, respectively) were
introduced as low-temperature binders. 3D ceramic parts with reason-
able dimensional accuracy and part definition, such as gears and casting
moulds, were successfully fabricated. The underlying reason for such a
feedstock arrangement can be explained as follows. As refractory mate-
rials, ceramics generally have very high melting points. Although as a
heating source, a high-power laser can potentially generate temperatures
Fig. 28. Complex ceramic parts produced by SLS: (a) Al2O3 parts with the assistance of quasi-isostatic pressing and final firing [211]; (b) 3YSZ parts after SLS and
after combination with pressure infiltration (PI)/warm isostatic pressing (WIP) and final firing [212].
13
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
high enough to trigger the densification process, which is a solid-state
diffusion-dominated process, and sufficient exposure time is also needed
to achieve the desired densities, it remains exceedingly difficult and
impractical for the local densification of ceramic powder to occur.
Therefore, SLS of ceramics is challenging, in that measures should be
taken to lower the target temperature used to bond the powder and thus
to facilitate the densification. A viable solution is to coat or mix other
materials of lower melting/softening points acting as binders on/in the
matrix powder. In this way, the laser beam heats the powder bed surface
and the binders melt and form a glassy phase around the ceramic par-
ticles for bonding. An additional advantage is that these materials are
also more tolerant to temperature gradients. It is worth noting that the
binder can be either organic (e.g. polymers) [202–204] or inorganic (e.g.
metal-based low-melting materials and glass) [201,205–209]. After the
SLS process is complete, the organic binder contents are subjected to
further decomposition and removal by high-temperature firing in a fur-
nace, so that the final ceramic parts can be obtained. Inert atmospheres
(e.g. N2, Ar) should be maintained during the SLS process to prevent
possible oxidation of the binder contents. With regard to the inorganic
binders, however, these cannot be removed by firing. The binders thus
either remain in the final parts or react with the matrix powder to form a
secondary phase.
Two major concerns in the SLS of ceramics are the high shrinkage of
and the high porosity remaining in the final parts. Shahzad et al. [210]
reported the SLS of submicron alumina composite microspheres con-
taining up to 50 vol% Al2O3, coated with polyamide-12 (PA12, soft-
ening point ∼125 °C) by a phase inversion process. The composite
microspheres showed good flow characteristics, although the final
sintered density of the produced parts was less than 50% of the theo-
retical density owing to the persistent low powder bed density caused
by the intersphere space (i.e. remaining all the way through the steps of
powder spreading, laser sintering and final firing). The final ceramic
parts are shown in Fig. 28(a).
It is known, however, that structural ceramics must be made almost
fully dense so that their optimal mechanical performance can be
achieved. To maximise the density of the final ceramic parts, infiltra-
tion/isostatic pressing can be used, along with SLS [213]. Fig. 29 shows
a general guideline flowchart of the various stages in the processing of
ceramic parts to improve their porosity and mechanical strength.
In this way, Shahzad and co-workers [211,212,214–216] later de-
monstrated the fabrication of complex ceramic parts with improved
densities. Starting with Al2O3–PA composite microspheres, Al2O3 parts
with an increased density of up to 94% of the theoretical value were
obtained using SLS assisted by quasi-isostatic pressing (QIP) at elevated
temperatures [211]. In another study [212] of the SLS of Al2O3–PP
(polypropylene, melting point ∼160 °C) composite spheres, after post-
processing by pressure infiltration with 30 vol% alumina powder-based
ethanol suspension and warm isostatic pressing (WIP) at 135 °C and
64 MPa, the green density increased from 34% to 83% and the final
density increased from 64% to 88%. In the same way, a final density of
3 mol Y2O3-stabilised ZrO2 (3YSZ) parts produced by SLS combined
with WIP was reached, which was up to 92% of the theoretical density,
although it generated large linear shrinkage of > 35%. The parts
Z. Chen et al.
Fig. 29. Flowchart of SLS processing of ceramic parts combined with other treatments (processes marked with an asterisk (*) are optional).
produced are shown in Fig. 28(b). The significant shrinkage caused by
densification after a series of treatments is readily seen.
PDC parts were also produced using SLS by Friedel et al. [217] using
the starting feedstocks of a binary material system, i.e. SiC powder as a
filler (loading up to 60 vol%) and PMS (melting point ∼60 °C) powder
as a pre-ceramic precursor. It was claimed that final densities of 50%
and ∼100% without and with liquid silicon vacuum infiltration at
1500 °C, respectively, were reached. Only ∼3% linear shrinkage was
induced after firing, with the bending strength dramatically increased
from 17 MPa for the green part to 220 MPa for the final part. The much
lower green strength was thought to be caused by a porosity of 50 vol%
and by microcracks in the SiOC matrix, although no porosity or cracks
were detected in the final part. The turbine wheel prototype fabricated
after each treatment step can be seen in Fig. 30.
Like its counterparts, ceramic SLS has also become increasingly
popular in biomedical applications, particularly in the fabrication of
customised complex and highly cellular biocompatible scaffolds for
tissue engineering. These fabrications generally involve high volume
fractions of binder phases of up to 60 vol%, and so geometrical accuracy
and surface roughness are not strictly required for these applications,
Fig. 30. SiOC/SiC turbine wheel produced: (a) after SLS; (b) after firing; (c) after infiltration with silicon [217].
14
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
although macro-porous structures are often customised in a controllable
manner. Examples include bone implants made by ceramic–polymer
blends, such as hydroxyapatite–tricalcium phosphate (HA-TCP) [204],
hydroxyapatite–polycarbonate (HA-PC) [218], hydro-
xyapatite–polyether ether ketone (PA-PEEK) [203] and silica–polya-
mide (SiO2-PA) [219]. Ceramic–glass composites have also been in-
vestigated for the fabrication of biocompatible scaffolds, such as
hydroxyapatite–phosphate glass [220], apatite–mullite [221,222] and
apatite–wollostonite [208]. In these applications, the low-melting point
polymers and glasses served as liquid-phase binders during SLS to fa-
cilitate densification. Examples of fabricated calcium phosphate–poly-
hydroxybutyrate-co-hydroxyvalerate (CP-PHBV) scaffold micro-
structures are shown in Fig. 31 [223].
It is worth pointing out that the properties of the parts produced by
SLS are affected by a number of factors associated mainly with the
feedstock materials and laser–material interactions. On the one hand,
good flow characteristics are required for the matrix and binder pow-
ders, which are better for particles of spherical shape and micrometre
size [224]. Moreover, the amount of binder may strongly influence the
mechanical performance of the green composite parts [225]. It is
Z. Chen et al.
preferable to have a low fraction of binder since the final porosity is
also dependent on the amount of binder. Generally, matrix powder
coated with binder generates a higher part strength than mixed ma-
trix–binder systems owing to the inhomogeneous distribution and
segregation of the binder in the latter [226]. The assistance of isostatic
pressing and infiltration described earlier can also help to reduce the
packing porosity and hence increase the final part density. Efforts have
also been made to improve the part density by modifying the feedstock
form. Instead of the conventional powder-based feedstock ceramics
used for SLS, a slurry-based form was also developed by Tang et al.
[227] to fabricate high-density (98%) Al2O3 parts with polyvinyl al-
cohol (PVA) as a binder. Such a high density was attributed to the high
dispersion and homogeneity of the slurry-based powder bed. On the
other hand, SLS is a very complex process due to the underlying me-
chanism involved in the reaction between the laser beam and the ma-
terials. There are various dynamic conditions appearing at the localised
microscopic interaction volumes that have to be considered during the
rapid laser fusing process. Such a process ultimately influences the
microstructures, mechanical performance and geometries of the parts
produced. One of the crucial factors is the energy of the laser applied to
the powder bed during SLS, which is directly associated with the laser
power and scanning speed. The laser energy required relies on the
mixed powder composition, the thermal properties of the powder, such
as the melting point and thermal conductivity of the material, and the
packing porosity of the powder bed. Too low a laser energy leads to
insufficient fusion of the binder, generating poor bonding of adjacent
layers, resulting in low green strength, while too high an energy results
in excessive melting and evaporation of the binder, thus causing da-
mage to and geometrical inaccuracy of the part [217,227].
To sum up, a broad range of material combinations can be used with
the SLS technique, allowing for a comprehensive range of applications
in functional and structural ceramics fabrication. Moreover, the sup-
port-free building process of SLS also enables the realisation of geo-
metrically controllable complex/porous ceramic parts. Like other 3D
printing methods supplied with vat/bed-based feedstocks (e.g. SL, DLP,
TPP and 3DP), ceramic SLS is also an indirect multistep process in
which a sacrificial binder material is used for the bonding of ceramic
particles and then removed by debinding in a subsequent high-tem-
perature firing process. Therefore, ceramic SLS is not capable of pro-
ducing fully enclosed structures as the untouched materials cannot be
drained. Although the disadvantages of ceramic SLS include low re-
solution, poor surface finish and porous microstructures within the
fabricated parts, it is acceptable for most applications, particularly in
the tomography-assisted fabrication of scaffolds for biomedical en-
gineering purposes. Moreover, additional processing steps, such as in-
filtration and isostatic pressing, should be considered to enable the
fabrication of structurally sound parts with desirable strength and little
geometrical distortion.
3.3. Selective laser melting (SLM)
Often considered as a variant of SLS, the SLM process was developed
at the Fraunhofer Institute for Laser Technology (ILT) in Germany in
15
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
Fig. 31. (a) Digitally designed complex 3D
cellular models; (b) final CP-PHBV porous
structures made with SLS; (c) 3D model of a
human bone reconstructed by CT and pro-
cessed into a porous scaffold with cubic units;
(d) final CP-PHBV scaffold made with SLS; (e)
SEM image of one layer of the fabricated scaf-
fold; (f) cytocompatibility tests: morphology of
SaOS-2 cells cultured for seven days on the
scaffold [223].
1996, resulting in German patent DE 19649865 [228], later filed in the
USA in 1997 [229]. It proceeds in almost the same way as SLS except
that it is a time-saving, one-step powder bed fusion by full melting,
which uses laser sources with much higher energy densities and re-
quires no secondary low-melting binder powders. Thus, SLM can pro-
duce nearly fully dense homogeneous parts without post-treatments
owing to its ability to fully melt the powder into the liquid phase, en-
suring rapid densification, instead of heating up the powder to a spe-
cific point where the particles are partially melted and fused together as
in SLS. The technology was originally developed to produce solid parts
from metal powders (e.g. aluminium, copper and stainless steel) and
has now been extended to the increasingly used advanced alloys, par-
ticularly for the production of lightweight parts for the aerospace in-
dustry [230]. Stronger functional and end-use production parts can be
produced using SLM with lower porosity and superior control over the
crystal structure. A schematic diagram of the SLM process is shown in
Fig. 32.
SLM is one of the most rapidly growing 3D printing techniques,
particularly in the metal forming field. This is mainly attributable to its
ability to manufacture strong and durable metal parts in a single-step
process, where the final shape and properties of the parts can be ob-
tained simultaneously. The application of SLM to a ceramic powder
involves full melting of the powder to form a solid part by high-energy-
density laser scanning layer by layer, without binders or post-sintering
owing to the full melting and fusion of the powder. Thus, complex parts
of higher purity, density and strength are expected to be produced in
less time. SLM is considered to be the only 3D printing process that
offers the possibility of manufacturing ready-to-use ceramic parts with
full density, high strength and complex net shape from ceramic powders
in a single step. The overall quality of an SLM-produced ceramic part is
influenced by many factors, such as feedstock properties, fabrication
parameters, fabrication position and orientation, post-processing and
the physical and chemical properties of the interaction in the fabrica-
tion process, including the interaction of the energy source and the
materials. One of the most important fabrication parameters is the slice
thickness, which may influence the production time and the surface
roughness of the part. A smaller slice thickness reduces the surface
roughness but at the same time leads to longer building time, whereas a
larger thickness may cause a significant stair-step effect. The slice
Fig. 32. Schematic diagram of the SLM process with preheating of the powder
bed.
Z. Chen et al.
thickness relies on the fusion depth, similar to the penetration depth in
the SL process. The fusion depth is directly related to the material
properties as well as the laser–material interaction. An optimal com-
bination of processing parameters may exist for balancing the overall
quality of the fabricated part.
SLM of ceramics, however, is much more difficult than that of me-
tals and other composite materials; thus, not much development has
been achieved in the ceramic forming field. During the SLM process,
laser processing parameters are crucial to the quality of the fabricated
parts. Problems such as the balling effect may occur with insufficient
energy input, whereas excessive amounts of energy would result in
spattering of the powder [231]. However, direct melting involves an
extremely high-temperature interaction between laser and powder, the
very short period of interaction leading to large temperature gradients
within small volumes of material. One of the most significant problems
arising from the SLM process is the thermal stress induced by extremely
short laser–powder interaction times, namely, the drastic heating and
cooling rates upon each laser scan [232]. Cracks and distortions are
most likely to form in the sintered parts owing to such thermal stresses
as a result of the limited thermal shock resistance of the ceramic ma-
terials. In 2007, Shishkovsky et al. [233] from the École Nationale
d’Ingénieurs de Saint-Étienne (ENISE) in France reported the fabrica-
tion of ZrO2 parts using SLM, while defects such as cracks and large
open pores developed (Fig. 33(a) and (b)). Mercelis et al. [232] in-
vestigated experimentally the origin of the residual stresses in the SLM-
fabricated parts, and a simple theoretical model was developed to
predict residual stress distribution. It was found that the scanning
strategy has a large influence on the residual stresses and that the
stresses are larger perpendicular to the scan direction than along it.
The short interaction time may also lead to insufficient melting,
resulting in large residual porosity and poor surface quality in the
fabricated part. Deckers et al. [234] fabricated Al2O3 parts using SLM,
with only an 85% density reached. The large residual porosity was at-
tributed to the incomplete melting of the material during laser scan-
ning, although the layer deposition and laser scanning parameters were
carefully optimised. Bertrand et al. [235] reported the SLM of pure
ZrO2–Y2O3 powder. The fabricated parts possessed a very low density of
56%, and no improvement could be achieved using further heat treat-
ment in a conventional furnace. The fabricated part is shown in Fig. 34,
along with an SEM image of the highly porous microstructure. The
rough surface finish and porosity are clearly apparent. The increase in
the powder bed packing density may help to enhance the final part
density, as suggested by the authors.
Several modified 3D printing methods derived from SLM have been
shown to be capable of fabricating ceramic parts, such as slurry-based
SLM [236,237] and laser-engineered net shaping (LENS) [238,239]. To
increase the powder bed density for SLM so that the disadvantages of
low sintered density and cracking may be prevented, other forms of
powder packing have been developed instead of dry powder deposition.
Among them the slurry form appears to be promising and has the ad-
vantage of a more homogeneous and highly packed nature. Stable
slurries loaded with an Al2O3–SiO2 powder mixture (up to 63 vol%) and
Fig. 33. Surface morphology of the sintered ZrO2 part showing: (a) cracks; (b) open pores; (c) ZrO2 objects produced by SLM [233].
16
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
water with a high fluidity have been prepared by Gahler et al. [237]
and then deposited layer by layer using a doctor blade as in tape casting
before drying. The fabricated parts possessed a smooth surface and
densities of up to 92% due to the liquid-phase formation of SiO2.
Subsequent developments have successfully fabricated various types of
structural porcelain objects without achieving fully dense micro-
structures [240,241].
In LENS, the feedstock powder is deposited coaxially to the desig-
nated laser spot area as the beam moves so that the molten pool is
formed immediately [242]. Dense Al2O3 in the shape of cylinders, cubes
and gears were fabricated successfully by Bella et al. [239] using LENS,
resulting in anisotropy of the obtained mechanical properties. A relative
density of only 94% was achieved. Heat treatment failed to alter the
strength and anisotropy, but did increase the grain size from 6 to
200 μm. Cracks developed along the columnar grain boundaries when
tensile loads were applied. Fully dense simply shaped Al2O3–YSZ parts
with fine-grained microstructures were fabricated by Niu et al. [243]
using LENS. The eutectic spacing of the lamellar colony reached 100 nm
owing to the rapid melting/solidification process. The mechanical
performance was comparable with those prepared by traditional di-
rectional solidification. However, the surface quality and dimensional
accuracy remain unsatisfactory.
Optimisation of the laser processing parameters only is thought to
have little effect on the mitigation of such thermal-gradient-induced
problems. Studies [244,245] have demonstrated that preheating the
ceramic powder bed is effective in reducing the tendency for defects
such as cracks and distortions induced by thermal stress to form, as
shown in Fig. 35(a). In addition, simultaneous crystallisation during
solidification might yield a fine-grained microstructure, potentially al-
lowing for superior mechanical properties due to grain boundary
strengthening [246]. However, the high melting points of ceramic
materials require a preheating temperature above 1000 °C. An excessive
temperature close to the melting point would eventually result in a
larger molten pool size, which would cause unwanted outflowing into
the surrounding powder of the low-viscosity molten ceramic material,
thus increasing the dimensional inaccuracy (surface roughness
Rz = 60 μm and dimensional accuracy = 150 μm). To fabricate ceramic
parts with a fine and homogeneous microstructure, Wilkes et al.
[244,247] from the ILT in Germany used SLM to process pure ceramic
parts for potential applications in dental restorations based on the use
of eutectic mixtures of pure ZrO2 and Al2O3 powder. Thermal-gradient-
induced cracks were prevented by using a high-temperature preheating
system developed with a CO2 laser to preheat the powder layers (to
∼1700 °C) and an Nd:YAG laser for local melting. Fully dense parts
with a flexural strength of > 500 MPa were obtained without post-
processing, although the poor surface quality persisted. Thermal gra-
dients over the height of the part persisted, and only small-sized parts
(wall height < 3 mm) could be produced with top-down laser pre-
heating of the powder bed. Alternative preheating strategies, such as
bottom-up inductive preheating and diode laser selective preheating,
were developed to allow the fabrication of larger parts with further
minimised thermal gradients. The fabricated ceramic parts can be seen
Z. Chen et al.
Fig. 34. (a) 3D CAD model of a nozzle, (b) fabricated zirconia part and (c) SEM image of a cross section showing the high porosity [235].
in Fig. 35(c).
More recently, the resolution and surface roughness of ceramics
prepared by SLM were greatly improved by a modified method, referred
to as laser micro sintering (LMS) [248,249], based on the use of sub-
micron powder and a Q-switched near-infrared solid-state laser with a
wavelength of about 1 mm. The generation of fully dense parts made of
several types of ceramic materials (e.g. Al2O3 and SiC-based ceramics)
was successfully demonstrated, with resolutions down to a few tens of
microns and a surface roughness of a few microns, both of which had
previously been made to an order of magnitude higher with the con-
ventional SLM technique. The fabricated parts with very fine resolu-
tions and detailed features are shown in Fig. 36. However, it is only
practical to fabricate parts with very small volumes by LMS.
Even though much work has been done on the SLM of ceramics, the
applications of SLM-produced ceramic parts are still very limited. This
is mainly attributable to the generation of defects such as porous mi-
crostructures, rough surface finishes and low dimensional accuracy, and
densification to a non-porous, isotropic ceramic body is hard to achieve.
Therefore, further endeavours need to be made to improve the material
properties, fabrication process and post-processing, to achieve the
fabrication of truly defect-free, high-precision and fully dense ceramic
parts.
4. Bulk solid-based technologies
4.1. Laminated object manufacturing (LOM)
LOM was first reported by Kunieda in 1984 [250], then further
developed by Helysis Corporation in 1986 [251] and commercialised in
1991. It was originally developed to produce paper, plastic and metal
components. The process generally involves computer-controlled laser
cutting of as-prepared thin sheets of materials into cross sections ac-
cording to sliced digital CAD models and subsequent layer-wise adhe-
sion of one cut sheet on top of another, pre-coated with adhesive
agents, to form 3D parts. Bonding and lamination between adjacent
layers can be accomplished by real-time heating and mechanical com-
pression. A schematic diagram of the LOM process is shown in Fig. 37.
Fig. 35. Cross sections of ZrO2–Al2O3 parts produced by SLM: (a) without and (b) with preheating, with the arrows in (a) indicating cracks; (c) ZrO2–Al2O3
frameworks for dental restorations produced at a preheating temperature of ∼1700 °C [244].
17
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
The application of this technique to ceramics manufacturing was
first demonstrated by Griffin and co-workers in 1994 [252,253], based
on tape-cast alumina and zirconia green sheets. Continuous rolling of
long green ceramic sheets onto the working platform allows the pro-
cedure to be fully automated. Excess material surrounding the parts
being fabricated is removed layer-wise prior to lamination of each
layer. Finally, high-density parts can be obtained after further binder
removal and sintering at high temperatures.
Besides the first report by Griffin on the LOM of Al2O3 components,
a number of demonstrations have followed that were successful in
fabricating other structural ceramics, including SiC [254], Si/SiC
composite [255], ZrO2 and ZrO2/Al2O3 composite [256], TiC/Ni com-
posite [257], LiO2–ZrO2–SiO2–Al2O3 (LZSA) glass–ceramic composite
[258] and functional ceramics such as PZT for functional telescoping
actuators [259] and HA for bone implant preparation [260]. Some at-
tention has been focused on LOM fabrication of novel lightweight
ceramic parts based on pre-ceramic papers filled with ceramic powder,
such as Al2O3 and SiC [261–263] (Fig. 38(a) and (b)).
Notably, Rodrigues et al. [264] reported the use of LOM to fabricate
Si3N4 parts (Fig. 38(c)), with an average final density after sintering of
97% relative to the theoretical density as a result of an average volume
shrinkage of 40%. The microstructures and mechanical properties, such
as Young’s modulus, flexural strength and fracture toughness, measured
for the final parts were shown to be comparable to Si3N4 prepared by
conventional methods such as reaction-bonding, slip casting and pres-
sureless sintering [265,266].
In a more recent study, the LOM of ceramics has been demonstrated
with MAX phase Ti3SiC2 composite [267]. Again, a defect-free gear
with a linear shrinkage of less than 3% relative to the green state was
obtained, as shown in Fig. 39.
Other work has also been conducted that has concentrated on LOM
system and process improvement, such as the build time, working
parameters and surface roughness [254,268–270].
The advantages of this technique are the elimination of distortion
and deformation as a result of the low thermal stresses induced in the
manufacturing process [184]. However, the main disadvantages are
also directly related to such a process, since delamination, interfacial
Z. Chen et al.
Fig. 36. LMS of complex-shaped ceramic components made from: (a) Al2O3; (b) SiO2; and (c) SiSiC at micron-scale resolution [248].
Fig. 37. Schematic diagram of the LOM process.
porosities and anisotropic properties along the planar directions and the
building direction are the common problems associated with weak in-
terfacial bonding behaviours between layers [188,258,271]. The use of
LOM is also restricted, as only laminated sheets can be used in the
process. Like most other conventional 3D printing techniques, poor
surface quality could be another significant drawback for LOM, parti-
cularly when dealing with round-shaped surfaces. Attempts have been
made to address this problem by combining LOM with high-speed
cutting techniques [272].
Despite much attention being paid to research into the LOM of
ceramics, most of the above-mentioned studies were carried out several
years ago and by only a few groups. Although the LOM technique is
claimed to be capable of producing parts with complex structures, its
implementation in ceramics fabrication has mostly centred on simple
structures such as gear prototypes (as shown in the figures in this sec-
tion). Not much technological progress or applications have been re-
ported in recent years, however, owing to the complex geometry of
advanced ceramic components as well as their miniaturisation down to
the micron scale. These pose difficulties for the ceramics LOM process,
which generally produces parts at relatively larger dimensions with less
complex structures, as shown earlier.
4.2. Fused deposition modelling (FDM)
The FDM method, also known as fused deposition of ceramics
(FDC), is one of the most commonly used 3D printing techniques. It was
first developed by Crump et al., with a patent filed in 1989 [273], and
later commercialised by Stratasys Inc. in 1990 [274]. At present, open-
sourced consumer FDM machines are believed to have the largest unit
shipments among all types of 3D printers owing to their various ad-
vantages, such as simplicity in the building process, flexible unit size,
ease in use and DIY and, more importantly, the low cost of both
18
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
machines and feedstock materials [275]. Thermoplastic polymers
[276], including ABS, PC, PA and polylactic acid (PLA), in filament
form are the most frequently used materials for FDM 3D printing. In an
FDM process, the material filament is continuously supplied to and
heated within a moving nozzle at a temperature just above its melting
point so that it can be easily extruded via the nozzle to form layers.
Upon extrusion, the material solidifies immediately over the previously
printed layer. Like some other 3D printing technologies, the platform
then lowers so that the extrusion of the next layer can take place.
Supports can be built and removed after the part is complete. The
vertical dimensional resolution of the part is determined by the layer
thickness, which in turn depends on the nozzle size [277]. A schematic
diagram of the FDM process is depicted in Fig. 40.
In the past, the materials used for FDM have ranged from plastics to
metals and ceramics. It is clear that brittle ceramics cannot be shaped
into flexible and windable wires as feedstocks. As a result, for ceramic
materials to be used in FDM, composite filaments are prepared by
densely loading ceramic particles (up to 60 vol%) into thermoplastic
binders. Fig. 41 shows a ceramic–polymer composite filament prepared
using ABS as the matrix material filled with 3 μm barium titanate (BT)
powder up to 35 vol% [278].
After printing that is similar to the conventional FDM process is
finished, the printed ceramic part is subjected to binder removal and
sintering to achieve densification. The first application of FDM to the
fabrication of ceramics was reported by Danforth [279] at Rutgers
University in 1995 using Al2O3- and Si3N4-filled binder systems. The
final sintering densities were found to be unsatisfactory (75–90%)
owing to the presence of defects such as voids in the sintered parts.
However, no delamination was detected. Fig. 42 shows the very first
ceramic hardware made using FDM, along with a cross-sectional SEM
showing the filament-like surface roughness.
Growth in potential applications lies in the fabrication of functional
electronic components. Allahverdi and co-workers [280] have suc-
cessfully demonstrated a number of ceramic transducers of various
shapes fabricated using FDM (Fig. 43), with polymers/piezoelectric
ceramics (e.g. lead–zirconate–titanate (PZT) and lead–magnesium nio-
bate (PMN)) composites as feedstocks.
Fine ceramic (calcium phosphate) periodic woodpile structures with
spatial resolutions of < 100 μm were successfully fabricated using FDM
by Yang et al. [281] (Fig. 44). The lattices have precisely controlled
dimensions and multiscale internal hierarchical architectures. With
controlled pore structures on these scales, the lattices are expected to
provide customised biological, mechanical and geometrical require-
ments.
Novel FDM systems have been developed for multiple ceramic
fabrication [282,283]. Jafari et al. [283] have successfully
Fig. 38. Ceramic components fabricated by
LOM: (a) Al2O3 turbine rotor; (b) SiC gear
wheels [262]; (c) complex-shaped Si3N4 parts
[264].
Z. Chen et al.
Fig. 39. 3D Gear with MAX phase Ti3SiC2 fabricated by LOM: (a) green sample; (b) after sintering in Ar; (c) after silicon infiltration [267].
Fig. 40. Schematic diagram of the FDM process, with inset showing the heating
nozzle depositing ceramic feedstock.
demonstrated the use of four extruders to produce multilayer PZT
sensor components, with two types of soft and hard PZT ceramics in one
layer. Mechanical properties comparable with other processing routes
were achieved [284] for dense structural Si3N4 parts produced by FDM
using filaments of 55–60 vol% ceramic loading.
Current ceramic FDM applications, however, have shifted to the
fabrication of bioceramic scaffolds [285–289] and lattice photonic
bandgap structures [290,291]. The reason for this might be that bio-
medical components require less accuracy, and the rod shape (fused
ceramic/polymer filament) fits well with the need for 3D woodpile
lattice structures. Fig. 45 shows scaffold and bandgap woodpile struc-
tures made with PCL-HA and alumina, respectively.
There are a number of factors with respect to ceramic feedstocks
affecting the FDM process [184,292–294], including ceramic particle
size/distribution and dispersity in the filaments, the ceramic/binder/
additive ratios and the viscosity, and hence the flexibility, of the fila-
ments. The viscosities of the fused filaments should generally range
from 10 to 100 Pa·s, and ceramic particles should be well dispersed in
the filaments so that a constant and stable flow can be attained. De-
gassing in vacuum and centrifugation can be applied to minimise air
entrapment in the ceramic/binder materials. Fast solidification is
Fig. 41. (a) Photo of the kneaded ABS-BT feedstock; (b) ABS-BT composite filament sample [278].
19
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
desirable for preventing sagging of the filaments when spanning fea-
tures without support structures are manufactured, particularly in
highly porous parts [188].
Similar to the case of FDM for conventional plastic materials
[295–297], in the FDM of ceramics, the quality of the printed parts,
such as homogeneity, surface roughness, dimensional accuracy and
mechanical properties, also closely depend on the process parameters,
including rod width (fused ceramic/polymer filament), layer thickness,
building orientation, raster angle etc. Among the properties mentioned
above, surface roughness is the primary concern for FDM processed
parts. The main problem is the staircase effect, which is also regarded as
the major disadvantage of FDM, as can be easily found in printed
ceramic parts. This is predetermined by the size of the extruded fila-
ment, resulting in limited control in the z direction [287]. Despite the
fact that improvements in surface roughness have rarely been studied
for FDM of ceramics [298], lessons might be learned from the extensive
and inspiring work on the parameter optimisation of the FDM of plastic
materials [295,299–302].
5. Conclusions
In recent decades, research challenges and industrial needs have
promoted ceramics massively to be an exciting new area of application
for 3D printing technologies. In this review, a concise survey of the 3D
printing technologies used for ceramics fabrication has been presented.
Ceramic components with highly complex structures that are im-
possible to be fabricated using conventional manufacturing methods
can now be prepared via 3D printing techniques, thus demonstrating
their great potential and value. The state of the art of the numerous
major techniques now available for the fabrication of ceramic parts has
been discussed in detail and illustrated with representative examples.
Particular attention has been paid to the historical origins and evolution
of each method. A thorough comparison of these techniques is provided
in Table 2, with the pros and cons listed for the various aspects of
concern involved in each process.
Z. Chen et al.
Fig. 43. Various types of transducers made by FDM: (a) tube-array; (b) bellows; (c) spiral; (d) curved transducer; (e) telescoping; (f) radial actuators [280].
Fig. 45. Bioceramic scaffold: (a) photo of the artificial bone scaffolds made from PCL-HA using CT-guided FDM [288]; (b) SEM image of the structure; (c) photonic
bandgap (PBG): unit cell structure of alumina fabricated using FDM [291].
Strictly speaking, a 3D printing process represents only a forming
procedure involved in the many steps within the preparation route to
the final ceramic parts. Therefore, the desirable properties of the final
parts must also rely on the composition and microstructure, which are
determined by the materials and sintering process. It is suggested that
the integration of the 3D printing process with appropriate feedstock
preparation and required post-treatments (such as infiltration and iso-
static pressing) offers a unique possibility for further enhancing the
properties and performance of the parts, although these steps in the
operation lead to increased production times and costs.
20
Journal of the European Ceramic Society xxx (xxxx) xxx–xxx
Fig. 42. (a) Filaments filled with Si3N4 for FDM
processing and the ceramic parts fabricated
from them; (b) SEM image of the cross section
of a green part showing no delamination be-
tween adjacent FDM-produced lines and layers
[279].
Fig. 44. (a) Fine lattices with regular spacing;
(b) lattices with graded spacing structures; (c)
side view of the lattices [281].
Although powder-based fusion methods (i.e. SLS and SLM) have
been extensively researched and well established for both plastics and
metals, their use in the fabrication of 3D ceramic parts is still under
development. Successful part fabrication and structural control would
rely on an improved understanding of the dynamic interactions be-
tween laser and ceramic particles, layer deposition mechanism and
melting process, which still have plenty of room for further theoretical
and experimental investigations. The residual stresses caused by
thermal gradients under fast laser heating and cooling rates within the
ceramic parts remain a major factor for inducing defects such as cracks
Z. Chen et al. Journal of the European Ceramic Society xxx (xxxx) xxx–xxx

and distortions. Although preheating of the powder beds can help mi-
tigate these phenomena, the high melting points of ceramics impose a
greater demand on the fabrication process. The coarse surface finish,
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Structural ceramics

Structural ceramics

Structural ceramics

Structural ceramics
Structural ceramics
undesirable porosity and large shrinkage of ceramic parts after pro-
cessing also limit their areas of application.

Bioceramics

Bioceramics
In contrast, slurry-based photopolymerisation methods (i.e. SL, DLP
and TPP) for ceramics fabrication have shown more promise, in that
controllable feature resolution and surface finish with desirable me-
chanical performance can be achieved for the fabricated parts. A variety
Process cost

of commercial machines are now available on the market for the fab-
Medium

Medium

Medium

Medium
rication of complex 3D ceramic components. In particular, DLP ma-
High

High

High
Low

Low

Low
chines are much cheaper than SLM systems, which makes DLP more
favourable for widespread use. Therefore, photopolymerisation
Feedstock cost

methods have shown greater potential over powder bed fusion in the
manufacture of 3D ceramics parts.
Medium

Medium

Medium

Medium
The aerospace and medical industries are the two most promising
High

High

High

Low

Low

Low

markets for ceramic 3D printing. However, owing to their rigid and

high standards of safety acceptance, challenges such as compliance is-
sues arise and result in long certification and qualification periods. In
Medium

Medium

addition, in these cases, cost-effectiveness is no longer an advantage

Surface
quality

High

High

High

High

Low

Low

Low

Low

compared to conventional methods. High-end parts of low lot sizes and

high customisation usually yield a high cost per part. Compact and
porous parts can be obtained using IJP and 3DP. These methods are also
suitable for the fabrication of macro-porous ceramic lattice structures,
support
Manual

similar to the techniques of DIW and FDM. A significant benefit of 3DP

Yes

Yes

Yes

Yes
No

No

No

No
No

No

techniques lies in their flexibility to use a large variety of feedstock

materials in powder form, despite the limited surface finishes of the
fabricated parts. The effects of low density, poor accuracy and poor
Post-treatment

surface quality can be regarded as negligible and are likely to turn into
Debinding/

Debinding/

Debinding/

Debinding/

Debinding/

Debinding/

Debinding/

Debinding/

Debinding/
sintering

sintering

sintering

sintering

sintering

sintering

sintering

sintering

sintering

favourable features in the applications of bioceramic scaffolds.

Therefore, continual progress has been made in the fabrication of such
N/A

porous bioceramic components using the above-mentioned methods.

Despite the great progress made in the selection of usable ceramic
materials, the optimisation of processing parameters and post-proces-
Indirect

Indirect

Indirect

Indirect

Indirect

Indirect

Indirect

Indirect

Indirect
indirect
Direct/

Direct

sing, obstacles to the wider use of 3D printing in ceramics fabrication

still exist. Industrial mass production can be very challenging, and
ceramic components of larger size (e.g. a few metres) remain rare and
Medium

Medium

Medium

Medium

Medium

Medium
Speed

difficult to produce with 3D printing owing to the characteristic high

Slow

Slow

Slow

High

brittleness and low expansion coefficient of the materials. To extend the

applicability of 3D printing of ceramics and realise large-scale pro-
Resolution

μm–mm

μm–mm

μm–mm

μm–mm
μm–mm
nm–μm

duction of quality technical ceramic components to gain a significant

Comparison of the different 3D printing technologies used for ceramics fabrication.

mm

mm

industrial impact, it is advisable to base future advancement in the field

μm

μm

on material development and process control, most importantly with an

100 μm–100 cm

100 μm–100 cm

100 μm–10 mm

100 mm–10 cm

100 mm–10 cm
100 μm–10 cm

emphasis on improvements to the forming mechanism to allow near net

10 mm–10 cm

10 mm–10 cm

10 mm–10 cm
1 μm–1 mm

shape production of high-performance ceramic components at reduced

Part size

cost and in less time.

Acknowledgement
Power source

This work is supported by the Guangdong Provincial Department of

Thermal

Thermal

Thermal

Thermal
energy

energy

energy

energy

Education Youth Innovative Talent Project (2017KQNCX179), Key Project

Laser

Laser

Laser

Laser

Laser
Laser

Fund for Science and Technology Development of Guangdong Province

(2017B090911014), Shenzhen Peacock Plan Technology Innovation
Sheet lamination
Forming method

Binder bonding

Binder bonding
Polymerisation

Polymerisation

Polymerisation

Powder fusion

Powder fusion

Project (KQJSCX20170727101223535, KQJSCX20170327150948772),

Shenzhen University Startup Fund (2017035) and Shenzhen Fundamental
Extrusion

Extrusion

Research Project (JCYJ20150626090430369).

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