JMMP 05 00089
JMMP 05 00089
Manufacturing and
Materials Processing
Review
A Review on Printed Electronics: Fabrication Methods, Inks,
Substrates, Applications and Environmental Impacts
Jenny Wiklund 1 , Alp Karakoç 2, * , Toni Palko 2 , Hüseyin Yiğitler 2 , Kalle Ruttik 2 , Riku Jäntti 2 and Jouni Paltakari 1
in case of contact printing, while they are deposited onto the substrate typically through
nozzles in case of non-contact printing. Posterior to the printing process, it is often neces-
sary to conduct sintering/curing in order to reach the desired functional ink and substrate
characteristics. The inks, substrate and the printing technology along with the post printing
requirements must be carefully evaluated for quality, repeatability and life-time aspects of
the yield.
Although the requirements for the mass production of printed electronics with the de-
sired specifications are challenging, the current state-of-the-art for the materials, fabrication
processes and inspection technologies demonstrate an increasing trend in both repeatabil-
ity and functional performance [11]. Undoubtedly, continuous growth of biodegradable
and recyclable material portfolios for conductive, semiconductor and dielectric inks, and
synthetic and natural polymeric substrates are fostered by the printing and post-treatment
technologies, and optical inspection systems [12,13]. As a result, printing methods have
gained a ground for large area fabrication of flexible electronics including radio frequency
identification (RFID) devices; photovoltaic cells; organic light-emitting diodes (OLEDs);
thin film transistors (TFTs); diodes; displays; batteries; and sensors measuring temper-
ature, humidity and pH levels [14–17]. These developments demonstrate that reliable
and repeatable solutions for the mass production of printed electronics with well-defined
manufacturing standards will be available in very near future. In this study, we present the
printing principles and approaches by surveying the recent investigations in the manufac-
turing and material technologies, applications and environmental impacts.
2. Motivation
The rapid growth of the Internet-of-Things (IoT) is contributing to the evergrowing
interconnection of the digital world with the physical world. IoT is composed of a vast
number of smart objects with communications capabilities for transferring data through
wired or wireless communication networks. This includes, for example, various personal
smart devices, as well as traffic management, security and RFID systems. The smart objects
in general contain several sensing components (sensors) to acquire information about physi-
cal phenomena of interest and communication electronics to convey the data to the Internet.
As such, IoT enables novel applications and services on the cloud. Naturally, IoT is a new
frontier of information and communication technology (ICT) and sensor technologies.
IoT applications in healthcare, transportation, construction, leisure and sports verticals
enable transforming the objects from our everyday life into smart objects. This transforma-
tion inevitably requires the addition of semiconductors, sensors and related electronics,
which are designed to be discarded once the battery lifetime ends (possibly after a couple
of thousands charge–discharge cycles). Although adding intelligence to the devices in
everyday use is attractive and aids in digitalization of the physical world, it also shortens
their lifetime and becomes a major contributor to global e-waste [18]. The products that
might have lasted 15 years must be hence replaced every 5 years after such a transfor-
mation [19]. These periods become even shorter with the consumer intention towards
purchasing new models of fully-operational electronic products. In addition, more power
J. Manuf. Mater. Process. 2021, 5, 89 3 of 36
is needed to maintain this trend as the volume and use of such electronic devices keep
constantly increasing [20].
The consequences of the digital transformation and consumer behavior result in
massive amounts of e-waste produced globally [21]. For instance, in 2019, approximately
53.6 Mt of e-waste was generated and it is increasing at an alarming rate of 2 Mt per
year [22]. Out of these, only around 20–25% of e-waste are assumed to be formally recycled
while the majority is domestically dumped into the environment or illegally exported to
developing countries [23,24]. Despite the claimed percentages of formal e-waste recycling,
the absence of systematic procedures in the formal processes frequently ends up in the
landfill [25]. Improper handling of the matter, lack of environmental awareness and
consumer behavior cause irreversible impacts on both environment and human health [26].
Therefore, the current trend of adding intelligence into everyday objects and discarding
their environmental impact is not sustainable and requires alternative solutions that aims
at reducing the looming e-waste stream.
Printed electronics offer several benefits, which are not likely to be achieved with the
conventional electronics manufacturing. Kunnari et al. classified these benefits in terms
of ecodesign (efficient use of materials), minimization of energy consumption both in the
manufacturing and utilization phases, reduced use of hazardous substances, and improve-
ment of recyclability [27]. For instance, use of recycled and/or biobased materials to reduce
the use of raw/virgin materials as printed electronics substrates, and recovery of precious
metals used as inks have been a long-term objective and already accomplished by the
researchers in the field [28–32]. In addition, the metal inks have been under investigation
for depletion of precious materials and ecological aspects (both in raw material mining and
recycling) [33]. Therefore, separation techniques for metals from e-waste and development
of energy-efficient and environmentally friendly carbon based or polymer inks have been
investigated so as to replace or minimize the use of metal inks [34,35].
Printing technologies, as a part of the additive manufacturing umbrella, have been
extending electronics designers toolbox with access to various materials and ability to
apply unorthodox structures in their designs. While printing of all the components is
the ultimate aim of the electronics printing, most of the research activities are related
to design and manufacturing of individual electronic components. Especially, their low
manufacturing cost, large-area processability and lower carbon footprints compared with
their conventional counterparts has attracted significant interest from the scientific and
industrial communities. The printed electronic devices also provide favorable physical
characteristics, e.g., low weight, stretching, resistance to folding or bending, which can not
be realized with the conventional electronics [36,37].
In printed electronics, it is common for a device to be partly printed and partly
fabricated, as elaborated in the literature [38–40]. Various rigid components, such as
memory units, sensors and chips that are manufactured through conventional methods
can be combined with printed parts to form hybrid devices. However, with flexible and
stretchable printed electronics, the use of these rigid components impose challenges in
terms of mechanical and electrical integration. Although flexible interconnects and thinning
of the microelectronic components can be used for this purpose [13], a more promising
solution to this problem is to outright print these components.
As illustrated in Figure 2, researchers have reported passive, active and sensor printed
electronic components [3,7]. While passive components are designed and manufactured
based on electromagnetic properties of printed materials and shapes, active components
utilize nonlinear behavior of printed materials, and sensors are designed based on the
electro-mechanical features of the printed structures. A diverse range of active, passive and
sensor devices have been printed on thin and flexible substrates, which can be recyclable
or even biodegradable [41–47]. In the following subsection, recently investigated printed
electronic component classes are summarized.
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2.1. Sensors
Sensors convert various physical phenomenon, e.g., acceleration, temperature, mag-
netic field and capacitance, into electrical signals. As such, they are vital components
in a myriad of modern electronic across all application verticals. For instance, various
sensors are present in common household appliances, such as computers, security systems
and smartphones. In industrial manufacturing facilities, sensors are employed to moni-
tor ambient conditions and equipment parameters to ensure the quality of the produced
items. Sensors can be manufactured using printing technologies, since flexible, biodegrad-
able and stretchable sensing components compromise one of the most prominent area of
printed electronics.
Various printed sensors are reported in the literature, e.g., carbon nanotube (CNT)
based gas sensors [13], graphene-poly(3,4-ethylenedioxythiophene) poly(styrenesulfonate)
(PEDOT:PSS) humidity sensors [48], PEDOT:PSS based temperature sensors [49,50] and
active matrix sensor arrays printed on flexible substrate comprising organic TFTs, organic
photodiodes [13]. Recent developments on organic inks and lignocellulosic substrates have
demonstrated the printability of biocompatible and/or recyclable sensing devices. To name
a few, Kim et al. [51] fabricated entirely 3D-printed disposable ion sensor, Ling et al. [52]
explored the feasibility of inkjet-printed PEDOT:PSS/nanopaper-based touch sensor and
Guo et al. [53] demonstrated a 3D-printed pressure sensor composed of degradable and
fully recyclable thermoset elastomers. These sensors attest to their potential applications in
wearable and transient electronics. An example ensemble of printed sensors are depicted
in Figure 3, and a more comprehensive list is presented in Table 1. The tabulated works
have demonstrated that printed sensors may be designed to have performance metrics
comparable to their conventionally manufactured counterparts.
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Table 1. Collection of substrate and ink types used in various printed sensors.
Temperature sensor [60] Surface acoustic wave Lithium niobate (LiNbO3 ) Ag nanoparticle
(SAW)
Temperature sensor [61] Resistance Polyurethane (PU) plaster Graphene PEDOT:PSS solution
Strain gauge sensor [62] Resistance Buckypaper Ag nanoparticle
Poly-dimethylsiloxane
Strain gauge sensor [63] Resistance Ag nanoparticle & SBS/CB solution
(PDMS)
Figure 3. Printed sensors: (a) temperature sensors showing transparent property PEDOT:PSS (Reprinted
with permission from [50]. Copyright 2020 IEEE); (b) a CNT gas sensor array; (c) a resistive pressure
sensor array with test weights (Reprinted with permission from [13]. Copyright 2017 IEEE); (d) a
PEDOT:PSS based temperature sensor with silver nanoparticle electrodes (Reprinted from [49] under
CC BY 4.0 license).
Printed temperature sensors have been explored in detail by Rivadeneyra et al. [49]
and Lall et al. [50]. The temperature sensors studied by Lall et al. were printed in a Wheat-
stone configuration using silver, carbon and PEDOT:PSS on a flexible polyimide (PI)
substrate as presented in Figure 3a. In addition, a temperature sensor using this mate-
rial combination was also presented by Rivadeneyra et al., the purpose of which was
to generate a combination of both positive temperature coefficient (PTC) and negative
temperature coefficient (NTC) materials to measure a broad range of temperatures. As
can be observed in Figure 4, the resistance of PTC materials increases as temperature rises,
and vice versa; the resistance of NTC materials decreases when temperature increases.
Silver functions as a PTC material while carbon and PEDOT:PSS exhibit NTC behavior.
Rivadeneyra et al. [49] also studied specifically PEDOT:PSS based temperature sensors
printed on a flexible polyethylene terephthalate (PET) substrate (please, see Figure 3d), and
J. Manuf. Mater. Process. 2021, 5, 89 6 of 36
the effects of electrode spacing and fabrication methods on the thermal sensitivity of the
sensors. In recent years, fabric based NTC thermistors have been also gaining attention
due to the demand in wearable electronic textile industries. For instance, a recent work by
Li et al. [64] demonstrated that a novel low-temperature route can be used to print such
thermistors on polyester fabric, for which perovskite (Cs2 SnI6 ) ink can be used.
Figure 4. (a) Highly linear PTC behavior of silver throughout the test temperature range; (b) NTC
behavior of carbon; (c) NTC behavior of PEDOT:PSS. Note that carbon exhibits near linear NTC
behavior after an initial region of non-linear behavior (roughly from −40 ◦ C to −20 ◦ C). On the other
hand, PEDOT:PSS behaves near linearly initially from around −40 ◦ C to 70 ◦ C. (Reprinted with
permission from [50]. Copyright 2020 IEEE).
The work by Lall et al. [50] demonstrated that temperature sensors printed using
silver ink can reach to sensitivity values as high as 0.192%/◦ C temperature coefficient of
resistance (TCR). Furthermore, in the measured temperature range, resistivity of silver is
reported to behave in a highly linear fashion, as shown in Figure 4a. In contrast, the TCR
value of carbon is −0.048%/◦ C and −0.051%/◦ C with PEDOT:PSS. In addition, the NTC
of these materials changes non-linearly in some temperature ranges. The PTC and NTC
characteristics of just mentioned materials are given in Figure 4.
In the work by Rivadeneyra et al. [49], it was concluded that the sensitivity of printed
temperature sensors could be increased by altering the order of the fabrication steps.
Higher sensitivity values were obtained by first printing and drying the silver electrodes,
then printing and drying PEDOT:PSS and finally, sintering the sensor. In addition, it was
reported that the sensitivity of these sensors can be enhanced by a factor of 2.2 by increasing
the electrode spacing from 150 µm to 200 µm.
Strain gauge sensors are used across numerous industries for monitoring strains
caused by external forces and/or moments. As shown in Figure 5, such sensors are used
to monitor curing and exerted pressure during the manufacturing process and structural
integrity, and to monitor damage during the operation, i.e., for structural health monitoring
(SHM) purposes [65,66]. Recently, aerosol-jet printed CNT strain gauge sensors with CNT
onto buckypaper embedded in composite laminates demonstrated such sensor implemen-
tations in both resin flow and curing monitoring [62]. Thus, the effects of process defects
can be simply monitored during the entire life span of the structure, which gives a clear
idea about possible structural failures in advance. In a more recent paper by Wang et al. [63]
high sensitivity/low hysteresis screen printed strain sensors were also demonstrated. The
presented sensors have performance metrics comparable to their commercial counterparts.
This further indicates the great potential for printability of strain sensors.
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Figure 5. (a) Normalized impedance over time for vacuum and curing cycles for three types of resin;
(b) Printed strain sensor placed on glass fiber reinforced composite; (c) Results of impact hammer
bending of glass fiber reinforced composite with embedded printed strain sensor. (Reprinted from [62]
under CC BY-NC-ND 4.0 license).
Printed organic transistors can be also used for sensing slowly changing physical
phenomenon. For instance, a bacteria sensor, in which bacteria binding electrodes are inte-
grated with PEDOT:PSS transistor, was demonstrated by Demuru et al. [67]. Similar low
frequency sensors for measuring arterial pulse waves were reported by Laurila et al. [68], for
which the sensor was printed from piezoelectric poly(vinylidenefluoride-co-trifluoroethylene)
(PVDF-TrFE) and accompanied with entirely printed amplifier.
Figure 6. An illustration of an RFID system consisting of multiple RFID tags and an RFID reader
connected to a computer managing a database.
Currently, RFID tags can be manufactured in highly cost efficient manner using
printing manufacturing technologies. This opens up the possibility of using RFID tags, for
example, as part of packaging and other applications (please, see Figure 7), for which the
device has short life expectancy and is ultimately disposed. Literature on this subject has
shown that manufacturing of RFID tags is not limited to a specific printing technology,
and gravure, screen, flexographic and inkjet printing technologies have been effectively
used [38,39,81,82]. For instance,
In RF electronic hardware designs, power losses incurred in components and intercon-
nects need to be minimized, as these losses directly define the quality of the end-product. At
mm-wave frequency, inkjet printed interconnects have been found to outperform conven-
tional RF ribbon-bond interconnects, as reported by Eid et al. [83] and shown in Figure 8a.
The printed interconnects incur less losses at mm-wave frequency and generally are closer
to a continuous transmission line than the ribbon-bond interconnects. Furthermore, a
printed antenna targeted to operate at 3.5 GHz for 5G networks and at the frequency band
of wireless local area networks (WLAN), was demonstrated by Wang et al. [84] and shown
in Figure 8c. In addition to this, Jilani et al. [85] also presented an inkjet printed antenna
for mm-wave 5G, which was able to function in the 28 and 38 GHz frequency bands.
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Figure 7. (a) A printed RFID coil by the authors; (b) a fabricated RFID tag with an opening sensor
and force sensor as a part of the packaging [39]; (c) an RFID tag with light detection capabilities
printed on a flexible PEN substrate [40].
Figure 8. (a) Printed interconnect (above) and a ribbon-bond interconnect (below) (Reprinted with
permission from [83]. Copyright 2020 IEEE); (b) the structure for the embedded-on-package 5G
energy harvester (above) and printed device (below) (Reprinted with permission from [86]. Copyright
2019 IEEE); (c) Printed antenna for WLAN and 5G applications (Reprinted with permission from [84].
Copyright 2020 IEEE).
Figure 9. (a) Solar cell embedded into yarns (Reprinted from [97] under CC BY 4.0 license); (b) Trans-
parent organic solar cell (Reprinted with permission from [93]. Copyright 2020 American Chemical
Society); (c) Flexible perovskite solar cell (Reprinted with permission [94]. Copyright 2019 Royal
Society of Chemistry).
Currently, one of the most important and commercialized forms of the energy har-
vesters utilize photoelectric effects to generate electricity using photovoltaic cells (also
known as solar cells). They are mainly composed of supporting layer covered by pho-
tovoltaic or photoemissive cells and conductive transport grid [98]. The most popular
and commercial material for solar cells has been silicon due to its rigidity and physical
invariance for indefinite time frames. With a global market share of about 90%, the silicon
solar cells have power conversion efficiencies (PCEs) varying between 19 and 25% [99–101].
Printable solar cells, on the other hand, are promising candidates to harvest energy for
niche applications such as wearable textile electronics to charge low-power devices and
building-integrated systems to harvest energy from solar cells placed on roofs, windows or
facades of buildings [102]. In these applications, the fabrication scalability, light-weight,
flexibility and transparency are vital. In recent years, printed solar cells have gained a
momentum due to their simple preparation methods, low energy input/high-throughput
roll-to-roll (R2R) printing, and low carbon footprints. Recently reported PCEs of printed
solar cells is similar to commercial viable cells [103–110]. For the printable solar cells,
various photoactive materials have been implemented in the literature including hybrid
organic-inorganic materials like perovskites and organic conjugated polymer blends such
as poly(3-hexylthiophene) (P3HT) (as being donor) and [6,6]-phenyl C61-butyric acid
methylester (PCBM) (as being acceptor) [111–114]. Lab-scale investigations showed that
printed perovskite solar cells can reach up to PCE values comparable with those of silicon
solar cells, e.g., 16.6% PCE by Zhang et al. [115], 17.2% PCE by Schackmar et al. [116],
17.74% PCE by Li et al. [117], stabilized PCE of 18.5% PCE by Eggers et al. [118] and 19.6%
by Li et al. [119]. In addition to these developments, the printed organic cells developed
by Liu et al. [120] achieved 15% PCE. Very recently, Ma et al. [121] built a highly efficient
ternary system for as-cast organic solar cells with a 16.68% PCE while organic solar cells
developed by Cai et al. [122] reached up to 18.66% PCE.
In parallel with the emerging energy harvesting technologies, scientific advancements
in energy storage devices play vital role in a wide variety of low-power or self-powered elec-
tronics applications [123–125]. Recently, Xing et al. [126], Sundriyal and Bhattacharya [87]
and Aeby et al. [127] demonstrated flexible and disposable printed supercapacitors, also
known as electric double-layer capacitors (EDLCs), by integration of electrodes and separa-
tors onto lignocellulosic substrates such as paper. In the upcoming years, the research on
energy storage devices are expected to advance the current state-of-the-art and result in
more reliable, autonomous and recyclable IoT devices.
2.5. Displays
Printed organic transistors are attractive due to their flexibility, low manufacturing
cost and possibility to cover large structures or sheets cost efficiently. Those features have
fueled the success story of active matrix OLED (AMOLED) displays. Usage of organic
transistors in displays have been hindered by their low electron mobility. However, re-
cently, Mizukami et al. [128] demonstrated how DTBDT-C6 based organic TFTs (OTFTs)
J. Manuf. Mater. Process. 2021, 5, 89 11 of 36
can be used as a light source in printed displays. In their work, flexible color displays
were fabricated with inkjet printing technology (please, see Figure 10a). As depicted in
Figure 10b,c, a novel study on printed displays have been reported by Ivanov [129], in
which a screen printed electroluminescent matrix display were developed and described
in detail.
Figure 10. (a) A flexible color display (Reprinted with permission from [128]. Copyright 2018 IEEE);
(b) a screen printed electroluminescent matrix display integrated into a back pack; (c) a closer look of
the screen printed electroluminescent matrix display with the controlling module (Reprinted with
permission from [129]. Copyright 2018 IEEE).
3. Printing Technologies
The technologies used for printing electronic components are well-known in the
graphic arts. Some examples are gravure printing, flexography, offset printing, screen
printing and inkjet printing as depicted in Figure 11. These technologies are often grouped
into contact printing processes, which use printing master [130], contactless (non impact)
printing processes that do not need a master [131], and hybrid printing processes combining
different printing and deposition techniques. In a nutshell, all these processes are used
to deposit stacked layer structures, such as electrodes, conductive layers, isolating layers
for electronic components [132]. After deposition, the ink subsequently changes its phase
in the desired site [133–136]. The initial state, flow and phase change of the ink on the
substrate are mainly affected by the viscosity, density, surface tension, solvent evaporation
rate, solubility and curing characteristics of the ink, and wettability and permeability
of the substrate in use [137,138]. Moreover, multi-layer and multi-material nature of the
final device require compatibility and hence treatment of each layer to ensure the desired
function, e.g., minimal sheet resistance within a short-time span and without damaging
previously deposited layers. As exemplified in the previous section, typical printed devices
include sensors, batteries, capacitors, transistors, solar cells, memories, electroluminescent
structures, large screens, and light panels [34,139–148].
A well-known application of printed electronics is RFID systems where the antennas
can be printed. Printing the RFID antennas on flexible substrates is a very efficient solution
because it provides thinner, lighter and cheaper structures compared to the conventional
etching-based manufactured antennas. Gravure printing, offset and flexographic printing
methods are more commonly used for high-volume production needs, such as solar cells.
Offset and flexographic printing are primarily used for inorganic and organic conductors.
Gravure printing is suitable for printing high resolution and high quality structures such as
organic semiconductors and semiconductor/dielectric interfaces of transistors. In addition,
different printing and deposition techniques, such as gravure printing, via-hole screen
printing and electroless plating can be combined in hybrid printing processes [149,150].
In recent years, new printing processes have been also introduced. For example, Devaraj
et al. [151] created a novel printing process called as ‘form-fuse’. Through this process,
silver nanoparticle patterns are printed onto thermoplastic films using a large-area aerosol
jet printer with mask or a large-area inkjet printer without mask. In order to achieve the
desired geometrical shape, the printed patterns and substrate are vacuum formed. The 3D
patterns are then treated using flash light sintering in order to decrease the resistivity [152].
Moreover, a 4D printing technique using 3D extrusion and melt-electrowriting has been
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introduced by Constante et al. [153], which enables printing of anisotropic structures used
in biomedical applications.
The key properties and parameters of the different printing techniques are summa-
rized in Table 2. Inkjet printing has traditionally been better suited for R&D or special
applications, screen printing is excellent for stacking multiple thick prints, while gravure
and flexographic printing offer more opportunities for mass production of printed elec-
tronics [154]. Flexographic printing creates a thin printed layer with a feature size of 80 µm
and a throughput of 3–30 m2 /s. Offset and gravure printing provide similar features, the
latter being the fastest printing technology in terms of print press speed. Screen printing
and inkjet printing can give a larger layer thickness; inkjet printing up to 20 µm and screen
printing up to 100 µm even with a lower throughput of 2–3 m2 /s in screen printing and
0.01–0.5 m2 /s in inkjet printing.
is then transferred from the cells directly to the substrate in a printing nip under pressure.
Ink transfer is often improved by using an electrostatic assistance system (ESA) that creates
an electric field across the nip. The electric field assist in lifting the ink from the cells onto
the substrate. The ink layer is dried by evaporating the ink solvent with hot air [130,157].
Gravure printing is known for its high print quality and speed. For example, the
resolution is 20 to 400 lines/cm and the print speed is 13 to 16 m/s. Other benefits include a
simple printing process, accurate ink application, and flexibility in press design. Publication
presses are designed for fast printing of high-quality magazines, catalogs and brochures.
Print quality has further improved when laser engraving came more popular. However,
increased demand for short batches and personalization has reduced the market share
of gravure printing because the production of a printing cylinder is time consuming and
expensive [130,157].
3.1.3. Flexography
As illustrated in Figure 14, flexography uses soft and flexible printing plates in which
the pixels are raised on the top surface of the rest of the printing plate. The printing ink is
applied to the pixels through an anilox roll with small cells evenly engraved on the surface.
The surface of the anilox roll is applied with ink from the chamber and the excess ink is
then removed with a doctor blade. After formulation, the ink is located only in the cells of
the anilox roll. The ink is then transferred to the pixels on the surface of the printing plate.
The ink transfer takes place in a nip where the prevailing pressure allows the ink transfer
by improving the contact between the ink and the substrate. At the nip outlet, the ink layer
splits and some of the ink is transferred to the substrate. The ink layer is dried by blowing
hot air onto its surface. This causes the ink solvent to evaporate.
Flexography is used, e.g., for printing RFID antennas, batteries, organic electronic
circuits such as OLEDs and solar cells. OLEDs are used to make diode displays (tele-
visions, computer monitors) and lighting (diode lamps). Smart labels and thin films
printed on polyester film can be used, for example, to monitor temperature during drug
transport [158,159]. The resolution is typically 60 lines/cm and the print speed is 3 to
12 m/s. The biggest challenge is maintaining color saturation and density in fixed areas.
Flexography is suitable for a wide range of printing media. For example, non-porous and
porous substrates can be printed without problems.
Screen printing is a versatile and simple process for transferring ink to the surface of
substrates. The range of substrates is wide, from paper to ceramics in both sheets and con-
tinuous paths. The technology also allows printing on curved surfaces. Applications range
from art to large industrial applications, from small electrical components to multi-square
meter commercials, and from single-piece production to long print runs. Screen printing is
limited by relatively modest print quality. Screen printing is the oldest technology used
to print electronics. In addition, it is the cheapest, simplest and the most flexible printing
technology. It can be used, e.g., for printing electromagnetic enclosures, capacitors, mem-
brane switches or transistor electrodes. Screen printing has also been studied to print CNTs
and panels of graphene nanoparticles on polymer substrates [160,161] and flexible printed
supercapacitor structures comprising aqueous electrolyte and carbon electrode [150].
CS inkjet printing are displayed in Figure 17a. On the other hand, the high-resolution DOD
inkjet is primarily used for small-scale home and office printing, desktop publishing, and
high-quality wide-format printing and color coating. However, the print speed is slow. The
maximum resolution (2880 dpi) is up to five times higher than CS inkjet, and the droplet
size is also significantly smaller. In the DOD inkjet, every drop of ink hits the paper, and
no charging, deflection or recycling systems are required. The most common DOD inkjet
technologies are thermal and piezoelectric inkjets, which differ in formation technology.
Figure 17b shows the schematic of DOD inkjet printing.
Figure 18. Schematics of (a) pneumatic and (b) ultrasonic aerosol jet printing.
conductive material or a biometallic core-shell [42]. Gold is another easy to prepare metal
as a conductive ink, which is environmentally stable and requires relatively low sintering
temperatures. Besides, aluminum inks have been also synthesized; however, they have
high tendency for oxidation and chemically active characteristics.
In addition to the metallic inks, carbon-based conductive inks including CNT and
graphene have been also formulated, which are tailorable and used for specific applications.
For instance, metallic SWCNTs (m-SWCNTs) provide excellent stability, flexibility, light
transmittance, the conductivity of which increases with the thickness. Graphene has a high
conductivity, light transmittance, mechanical strength and elasticity; however, conductivity
increases and light transmittance decreases with increased amount of layers [148,158,166].
In recent years, conductive polymers have been also drawing attention due to their cost,
flexibility, light-weight and compatibility with aqueous and organic solvents. However,
they usually have lower electrical conductivity than metallic materials and their production
is challenging due to limited solubility, stability and processability. Moreover, the concentra-
tion of polymer inks is very low (1–6%), which also results in long drying times [148]. They
can be classified as conjugated polymers, polymer electrolytes, organic metal chelates or
charge transfer complexes. Among all conductive polymers, PEDOT:PSS has been the most
popular due to its high conductivity, moderate band gap, low redox potential, temperature
and humidity stability. PEDOT is insoluble but gains the soluble characteristics with PSS
as a dispersion. Even, the conductivity of PEDOT:PSS can be further improved by adding
organic compounds. Other commonly used conductive polymers in inks can be listed as
polyacetylene, polyaniline, polypyrrole, polyacene, polythiophene, polyparaphenylene,
polypyrrole and doped polyacetylene [158,166].
Conductive oxide ceramics have been also used as ink materials, which are usually
produced by doping in order to alter the cation or the anion lattice. Examples of doped
conductive oxide ceramics are antimony tin oxide (ATO), fluorin tin oxide (FTO), indium
tin oxide (ITO), aluminum zinc oxide (AZO) and gallium zinc oxide (GZO). Among
these materials, ITO is the most popular because of its superior conductivity; however,
it is a rare and expensive material [166]. Two types of ITO inks exist, which are sol-
gel and nanoparticle. The sol-gel ink has better conductivity but requires very high
sintering temperatures while the nanoparticle ink cannot form dense oxide films with high
conductivity [158].
polymer substrate materials in printed electronics [1]. PET is the most popular poly-
mer substrate, it has high optical transparency, flexibility, solvent resistance, low price
and dimensional stability in high temperatures [37]. PEN and PI on the other hand have
better heat resistance, but lower transparency and higher cost [158]. PC has high stabil-
ity, low weight and good mechanical properties, such as rigidity, impact resistance and
hardness [194].
PLA, PDMS, PVA, polycaprolactone (PCL), poly-lactic-co-glycolic acid (PLGA),
polyurethane (PU), polybutylene succinate (PBS) and polyethylene glycol (PEG) are ex-
amples of biodegradable polymers that can be used as substrate materials. PLA is a stiff,
transparent polymer, with a slow crystallization rate and low heat resistance, the mechani-
cal properties and heat resistance of which can be improved by, e.g., nucleation, change in
the stereochemistry or the use of additives [20]. PDMS is a highly elastic biocompatible
polymer, which could be used as a substrate in stretchable electronics [1].
As the manufacturing demand for wearable electronics has been increasing, the inter-
est in direct writing or printing of electronic devices onto textiles, such as polyester fabrics,
has become more important. Due to the commonly used high sintering temperatures, it
is unavoidable to damage such fabric substrates. Hwang et al. [195] demonstrated that
the use of low temperature sintering methods, such as intense pulsed light sintering, can
successfully overcome this problem while increasing the conductivity of printed patterns
on the fabrics. In Table 3, the glass transition temperatures, maximum service temper-
atures and other properties of some substrate materials are listed. Here, the maximum
service temperature refers to the highest temperature where the material can be used for
an extended period of time without notable problems.
Table 3. Glass transition temperature, maximum service temperature and authors’ comments about different recyclable and
biodegradable substrate materials. Here, the maximum service temperature refers to the highest temperature where the
material can be used for an extended period of time without notable problems [1,196].
5.1. Ink
Ink characteristics such as viscosity, surface tension, particle size and solid content (or
solid loading) have large impact on the printed electronics. To elaborate, the viscosity of
an ink specifies the resistance against the flow at a specific shear rate. As listed in Table 4,
different viscosities are required for different printing processes. The viscosity of an ink can
be modified; however, it is challenging to keep the same electrical properties with changing
the viscosity [166]. Increasing the temperature decreases the viscosity of the ink while
the solvent evaporation increases the viscosity [167,197]. The solvent in the ink can be
used to tune the viscosity of the ink. Additionally, increasing the dispersant concentration
decreases the viscosity of the ink [171]. Flexography, gravure and inkjet printing use low-
viscosity, liquid, inks, while offset, screen and pad printing use high-viscosity, paste-like,
inks [148].
Maximum particle size (nm) 15,000 15,000 10,000 1/10th of mesh 1/10th of 1/10th of
opening nozzle diameter nozzle diameter
Maximum preferred particle size
3000 3000 1000 100 50 50
(nm)
55 (ultrasonic
automization)
Maximum solid loading (wt%) 30 40 90 90 20
75 (pneumatic
automization)
There is a tension at the surface between a liquid and a gas, because of the asymmetric
attractive force between the molecules, this phenomenon is called surface tension. The
surface tension of the ink is important for the formation of drops, which also affects the
interaction between the ink and the substrate [171]. Polar liquids usually have high surface
tension, and nonpolar liquids low. An increase in the temperature or increase in solid
content can decrease the surface tension of an ink [167,197].
The functionality of metal particle inks improve with decreasing particle size [148].
Decreasing the particle size increases the surface area and increases the amount of stabi-
lizing agents required. Additionally, smaller particle size in the ink cause a high surface
to volume ratio, which lowers the required sintering temperature. Small particle size
and uniform size distribution in the ink produce higher viscosity inks and denser printed
patterns [167]. Furthermore, particle morphologies, e.g., nanospheres (NS) and nanowires
(NW), also affect both the electrical conductivity and energy needed for sintering. In their
recent studies, Dexter et al. [198] and Jahangir et al. [199] showed that mixing both NS and
NW can enhance the conductivity and reduce the energy needed for pulsed light sintering,
i.e., lower sintering temperatures. In addition, the investigations by Joo et al. [200] also
demonstrated the decrease in bulk resistivity while the NW weight content in NS:NW
mixture is increased up to 5%. As a matter of course, higher conductivity can be also
achieved by using inks with higher solid content. In the printing process, fewer gaps in
the pattern can be achieved with such inks. An increase in the solid content also leads to
viscosity decrease under shear stress, allowing the ink to flow more smoothly from one
surface to another while still preventing excessive spreading of the ink after printing. The
rheological behavior of the ink can thus be tailored by changing the solid content of the
ink [167].
J. Manuf. Mater. Process. 2021, 5, 89 23 of 36
5.2. Substrate
Different printed electronic devices require different properties such as flexibility,
high light transmittance, low surface roughness, light weight, low thermal expansion,
stiffness, heat resistance, low cost and low thickness [158]. The print quality is affected
by the surface roughness and porosity of the substrate [201]. High porosity and large
surface roughness can cause disconnected and nonuniform conductive patterns, due to ink
penetration. The disconnection of the conductive particles cause a decrease in conductivity.
Nevertheless, this can be avoided by using a coating for the substrate, increasing the
amount of conductive ink used or printing wider patterns [193,202]. Additionally, the
surface roughness has contingent impact on the conductivity of the printed pattern [170].
The surface roughness can be analyzed by studying the surface topography and the
cross-section of a sample. An atomic force microscope (AFM) or scanning electron micro-
scope (SEM) can be used to analyze the surface topography [203]. SEM can additionally be
used to study the cross-section of a sample after cutting the sample using a focused ion
beam (FIB) instrument. Other topographic measurement devices can also be used to study
the surface roughness. The porosity can be examined using a print penetration test or a
mercury porosimeter [170].
The performance of electronics is also affected by the surface energy and absorption
capacity of the substrate. The resolution of the printed pattern, ink penetration and ink
film thickness are affected by these surface properties. A decrease in porosity, decreases
the absorption, and a decrease in capillary absorption, decreases the spreading of the
ink laterally, which allows printing more accurate patterns. Substrate properties can be
modified for the purpose by using, e.g., chemical modifications, physical modifications
or coatings [193]. The surface energy can be calculated by testing several known liquids,
such as water, ethylene glycol and diiodomethane, on the substrate using an optical
tensiometer [170].
The dimensional stability of the substrate affect how the substrate reacts to changes in
the environment. Cracks and discontinuity in the printed patterns can be caused by poor
dimensional stability. The dimensional stability can be analyzed by exposing the printed
device to different environmental conditions, such as increasing humidity and temperature
and study the changes in the topographic and electrical properties [170]. Furthermore, the
substrate is often required to be thermally stable since some inks require high sintering
temperatures. The thermal stability can be tested by placing the substrate on a hotplate
and analyzing the changes in dimensions and color [203].
In some electronic applications, it is important to know the dielectric properties of the
substrate. In particular, the dielectric constant and dissipation factor must be known in
order to achieve the required precision. In general, the dielectric constant of the printed
device has to be low in order not to adversely impact high-speed electrical signals. The
dielectric properties of a substrate can be examined using methods, such as a microstrip
T-resonator, microstrip ring test or parallel plate capacitor [203,204].
The print quality is mostly affected by the equilibrium wetting, which can be deter-
mined by the contact angle (CA). The CA of a drop on a surface is the angle between the
tangents of the liquid–air and liquid–solid interfaces. The surface tension of the liquid,
the surface energy of the substrate and the environmental conditions, determine the CA.
If the surface energy of the substrate is higher than the surface tension for the ink, the
CA is small with an increased spreading of the ink. On the other hand, a high CA with
decreased spreading can be achieved by using a substrate with a lower surface energy than
the surface tension of the ink. A higher CA with decreased spreading results in thicker
patterns with higher resolution and a decrease in the line width [148,171,197].
The contact angle changes when it is observed over a longer time. An ink drop loses
mass due to evaporation, resulting in a decreased CA over time. It is important that the
evaporation rate is not too fast and allows for wetting and spreading of the drop. It should
not be either too slow with exaggerated spreading. A low advancing CA is required when
depositing individual ink drops on a substrate to form a uniform level high quality pattern.
Commonly the advancing CA is larger than the receding CA for most combinations of inks
and substrates, the difference between these is the CA hysteresis (CAH) [171]. If CAH is
high or CA is low, it is probable that the receding CA is zero [197].
Factors affecting CAH are porosity, surface roughness, chemical heterogeneity and
strong attractive interaction between ink and substrate. Surfaces with high porosity absorb
ink [148]. The surface roughness can increase the wetting and decrease the CA if the CA
is lower than 90°. On the other hand, if the CA is higher than 90°, the surface roughness
restricts the wetting of the surface. CAH is also increased by surface roughness. Addi-
tionally, a substrate with a high surface roughness and porosity can cause discontinuity
in the printed conductive pattern, which would cause a printed electronic device not to
function [136]. The effects of surface roughness can be minimized by surface treatments or
substrate patterning. Chemical heterogeneous materials have areas that are more wettable
and other areas that are less wettable, the receding CA is usually on the most wettable
areas, while the advancing CA is usually on the least wettable area. A drop and a substrate
that do not wet, but have a strong attractive interaction, can cause pinning of the edge of
the drop [197]. Additionally, high viscosity inks are usually more reluctant to spreading
compared to low viscosity inks [171].
by a decrease in the particle size used in the ink due to an increase in the surface-to-volume
ratio [42,171]. MOD inks usually require very high sintering temperatures, which limits
the choices for substrates used, and precipitation of metal [176]. Material properties can
also be improved by relieving internal stresses in solution-processed semiconductors, by
using annealing. Annealing is usually completed using an oven, hot air flow or hot plate.
The high temperatures used in annealing, limits its application [166].
The different temperatures required to thermally sinter various nanoparticle inks on
glass substrates are compared in Table 5. The silver nanoparticle ink clearly has the lowest
resistivity on glass substrate with a relatively low sintering temperature; however, there are
other factors affecting the sintering temperature and resultant conductive pattern resistivity,
e.g., the size of the conductive particle.
Table 5. Comparison of different sintering temperatures for different nanoparticle inks on glass substrates.
Photonic sintering transfer energy from a light source, such as flash lamps or lasers, to
the surface. Fast, high temperature and selective heating can be achieved by photonic sin-
tering, which is practical when using substrates that cannot withstand high temperatures.
The use of flash lamps enables effective sintering of the printed pattern with high-intensity
millisecond light pulses, increasing only the ink temperature without damaging the sub-
strate [200]. Intense pulse lamps can be used to sinter large areas (58 cm2 or larger) in
milliseconds using a broad wavelength spectrum (350–800 nm) [198,199,211]. Both contin-
uous and pulse lasers can also be used for sintering printed metal nanoparticle patterns.
High-resolution patterns can be achieved by using laser sintering, the laser beam can be
tuned for different patterns by adjusting the size and intensity [42]. UV-curing, on the other
hand, is commonly used for insulating and chemically stable materials, such as dielectrics
or insulators. Without heating, UV-curing can swiftly solidify the ink with sharp edges and
smooth morphology [166]. However, since plastic absorbs the wavelength range used in
UV-curing, it may cause damage to the plastic substrates [158].
High temperature plasma sintering and low pressure argon plasma sintering are also
selective sintering techniques [166]. Low pressure argon plasma is the most commonly
used plasma sintering method for printed patterns. The sintering starts from the surface
and continues into the bulk, and increasing the treatment time result in decreased resistivity.
Plasma sintering can be used for electronics printed on plastic substrates due to the ability to
use low temperatures but the penetration depth of the plasma limits the possible achievable
thickness of the printed pattern [42,158].
Microwave sintering is a very fast method for sintering metals. The penetration depth
of the radiation is, however, very small (approximately 1–2 µm at 2.54 GHz), which limits
the supported thickness of the printed pattern [158]. Metals with high thermal conductivity
can still use thicker patterns, due to the thermal conductance, and still form uniform
patterns [42,166].
Electrical sintering heats the printed metal pattern using electric current, caused by an
application of voltage over the pattern. The printed pattern is required to be somewhat
conductive already before the electrical sintering. This sintering method is low temperature
and very fast [42].
Chemical sintering is performed using chemical agents in order to provoke nanopar-
ticles to merge at room temperature. Oppositely charged polyelectrolytes are applied
to the metal nanoparticles to stimulate a spontaneous process where the nanoparticles
merge and create a conductive pattern. The polyelectrolyte can be added onto the substrate
J. Manuf. Mater. Process. 2021, 5, 89 26 of 36
prior to printing or onto the printed pattern after printing. Chemical sintering enables the
use of substrates sensitive to heat, such as plastics and paper. Negatively charged silver
nanoparticles can be chemically sintered using poly(diallyldimethyl-ammonium chloride)
(PDAC), as a positively charged polyelectrolyte [212]. Other examples of chemical agents
are ascorbic acid, hydrochloric acid (HCl), sodium chloride (NaCl), magnesium chloride
(MgCl2 ) and chloride ions (Cl− ) [42,136,166].
The differences in the resistivity of silver nanoparticle inks on glass and PI substrates
using different sintering methods are compiled in Table 6. In addition to the sintering
method, substrate and ink, the resistivity depends on the silver particle size, other materials
used in the ink and the printed pattern.
Table 6. Comparison of different sintering methods for nanosilver ink on glass and PI substrates.
Figure 19. Holistic overview for life-cycle of a printed electronics device. Operational energy is the
energy required to use the device while embodied energy refers to the consumed energy by the
processes associated with the production and end of life.
6. Conclusions
The present article provides a comprehensive review of advantages and limitations
of printed electronics in manufacturing, material, application and environmental aspects.
Based on the trends in industrial and scientific communities, and consumer markets, com-
monly used substrates, inks, and contact and non-contact manufacturing methodologies
are outlined in line with their applications. The recent developments in the printed elec-
tronics related materials and processes have resulted in not only low-cost/low-power
applications but also the creation of international multidisciplinary research teams for long-
term collaboration. Owing to these communities, there have been intense efforts to exceed
commercially viable thresholds and deliver end-products. Overcoming the limitations
related to their performance, durability and reliability, printed electronics will be expected
to replace their conventional counterparts and offer rapid and affordable manufacturing
with less environmental impacts.
Printed electronics are foreseen to be more accessible and available in our daily lives,
which will be one of the gateways towards a digital 21st century. Printed components are
progressively utilized not only in consumer electronics but also in the fields of energy,
biomedicine, transportation, construction and agriculture. Consequently, automation,
communication, sensing and monitoring, data collection and transfer electronics will be
affordably and autonomously manufactured with minimum demand for human labor and
fossil-based energy.
Author Contributions: Conceptualization, J.W., A.K. and H.Y.; Coordination, A.K. and J.W.; Writing—
original draft, J.W., A.K., T.P., H.Y., K.R.; Writing—review and editing, J.W., A.K., T.P., H.Y., K.R., R.J.
and J.P. All authors have read and agreed to the present version of the manuscript.
Funding: The authors gratefully acknowledge the funding from Academy of Finland BESIMAL
project (decision number 334197). J.W. also acknowledges the funding from Jenny and Antti
Wihuri Foundation.
Data Availability Statement: Not applicable.
Conflicts of Interest: The authors declare no conflict of interest.
J. Manuf. Mater. Process. 2021, 5, 89 28 of 36
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