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Received: 12 November 2021 Revised: 20 January 2022 Accepted: 22 January 2022

DOI: 10.1002/pen.25918

REVIEW ARTICLE

A review on in-mold electronics technology

~o1 | Fernando M. Duarte1 | Júlio C. Viana1


Mariana Beltra | Vitor Paulo2

1
IPC—Institute for Polymers and
Composites, University of Minho,
Abstract
Guimar~aes, Portugal In Mold Decoration (IMD) with printed electronic films combines the printed
2
GLN Innovation—Grupo Manuel functional film with the IMD process, creating a product with embedded elec-
Champalimaud, Leiria, Portugal
tronic functions that requires much less space compared to previous technolo-
Correspondence gies. In Mold Electronics (IME) is a process of integrating printed decorations
Júlio C. Viana, IPC—Institute for and functional electronics with IMD (i.e., thermoforming and injection mold-
Polymers and Composites, University of
Minho, Campus de Azurém, 4800-058
ing), resulting in 3D-shaped objects with embedded electronic functions. This
Guimar~aes, Portugal. technique is a field of recent large technological and scientific interests due to
Email: jcv@dep.uminho.pt its wide application, aesthetically appealing, and durable and lighter functional
Funding information products. This paper reviews the state-of-the-art of IME technology, resorting
European Social Fund (ESF), PT2020, to scientific research work performed and its main outputs, compiling and
Grant/Award Number: I&DPIIMIO -
analyzing the main knowledge and achievements on the process up to date.
POCI-01-0247-FEDER-042832; FCT -
Fundaç~ao para a Ciência e Tecnologia, First, an overview of the IME process steps is given, as well as, its components,
Portugal, Grant/Award Numbers: UIDB/ main applications, advantages, and drawbacks. The main IME printing tech-
05256/2020, UIDP/05256/2020
nologies are listed, and the relevant material parameters of the foil and of the
conductive inks for the printing process are also discussed. The effects of the
thermoforming and injection molding steps on the foil behavior and final
product are also addressed. Main challenges still to overcome on the IME tech-
nology are presented.

KEYWORDS
injection molding, processing, thin films

1 | INTRODUCTION assemblies.[2] Very low viscosity and low melting point


polymers are generally used to reduce the negative effects
In general terms, In-Mold Electronics (IME) is a process of high temperatures, high pressures, and high shear
for embedding electronic components/devices/functions stresses (due to polymer melt flow) on the electronic
inside thin 3D injection molded polymeric parts, by plac- devices that can be therefore damaged. This approach
ing them inside the mold and over-molding with a poly- aims mainly at protecting electronic devices from acci-
mer. Electronic components/devices/functions can be, dental loads, dirt, humidity, and water, facilitating the
for example, electrical components such as, sensors, assembly of electronic elements into polymeric parts.
LED, electrical circuitry, chips, PCB (printed circuit More recently, and due to technologies evolutions
board), displays, touch bottoms, antennas, etc. (Figure 1). and maturations, IME has adopted a different meaning.
For example, a PCB can be placed inside a mold and a This occurs due to developments of the printed electron-
low viscosity polymer can be over-molded.[1,2] Typically, ics (PE) and in-mold decoration (IMD) technologies. PE
this has been done by a low-pressure molding process, has gathered attention from the scientific community
where a very low viscosity thermoplastic polymer is used and industry due to the pairing of functional inks with
for over-molding and encapsulation/protection of PCB printing technologies. Still, the high-level integration and

Polym Eng Sci. 2022;1–24. wileyonlinelibrary.com/journal/pen © 2022 Society of Plastics Engineers. 1


2 BELTRÃO ET AL.

FIGURE 1 Common materials and respective fabrication processes used for IME

the manufacturing throughput remain as technological perfect and the printed layer is occasionally not uniform,
challenges, along with the development of high- all resulting in a high part rejection rate.
resolution printing technologies and the optimization of IMD with printed electronic films combines the
compatible functional inks.[3] Printing methods such as printed functional film with the IMD process, producing
inkjet, screen, and gravure printing are commonly a finished product with embedded electronic functions
applied to manufacture electronic components/devices. that requires much less space compared to previous tech-
Each printing method requires different ink parameters nologies based on PCB. This is IME, a process of integrat-
and offers distinct resolutions and thicknesses of the ing printed decorations and functional electronics with
printed patterns.[3] Functional inks include conductive, IMD (i.e., thermoforming and injection molding). The
semiconductor or dielectric inks that are being developed results are 3D-shaped objects with embedded electronic
based on metallic micro/nanoparticles, such as Ag, Au, functions.
Ni, Cu, C allotropes, organic materials, for example, con- IME is a technology that enables the development of
ductive polymers, dielectric ceramics, and polymers. structural electronics, where the electronics are inte-
Originally, PE is related to organic or polymer electronics grated into the structure of the polymeric part, rather
that use one or more inks made of carbon-based com- than being attached to it or connected with wires. It
pounds.[4] As demand for wearable devices and thinner should not be confused with molded interconnect devices
electronics expands, PE are being used to form flexible (MID) that is an injection molded part with integrated
keyboards, antennas, electronic skin patches, etc. In electric circuitry and mounted SMD (surface mounted
short, PE is one of the fastest growing technologies nowa- devices). MID combines a polymeric structure (housing)
days and it is becoming invaluable to several industries with electrical circuitry into a single part by selective
including healthcare, aerospace, and transportation. metallization. It is based on the development of struc-
IMD technology is a mature technology for the deco- tured metallization of polymers allowing new circuit
ration of polymeric parts.[5,6] In IMD, an aesthetic film, carrier designs over polymeric parts. All these tech-
printed with graphic inks of high color quality, is over- niques led to recent developments of the electronic
molded by a polymer. The integration of part decoration devices (Figure 2), moving toward the next generation
with complex contours in the injection molding process of PCB-less electronic applications.[7,8]
has benefits, such as the elimination of post-molding Regarding the commercial progress of IME, the mar-
operations, the high definition of the decorative pattern, ket has been ranging from simple devices for wearable
the improved adhesion quality, and the possibility of technology, automotive light heating, to more complex
using combinations of decorations and textures.[3] How- sensors and displays for HMI (human machine interface).
ever, there are disadvantages associated with this tech- The first commercial product was a Ford overhead con-
nique. For instance, the pattern resolution may not be sole of a car interior, released around 2012/2013, but
BELTRÃO ET AL. 3

structural electronics, including the IME process. A


report published by IDTechEx, in March 2020, previews
that this process can become a market bigger than $750
million by 2028.[9]
This paper gives an overview of the state-of-the-art in
IME, along with used functional materials (functional
inks and polymeric substrates), main printing technolo-
gies for functional films and its limitations, the pertinent
effects of thermoforming and injection molding on func-
tional device design and performance. Finally, main
issues to solve and still open points are highlighted.

2 | A V A I L A B L E T E C HNO L O G IE S
F I G U R E 2 Techniques for integration of electronics in
AND APPLIC ATIONS
polymeric molded components
IME technologies integrate several technologies already
mature separately: IMD, IML (both already integrating,
unfortunately the product was withdrawn from the mar- printed decorative films, thermoforming, and injection
ket. Recently, a remote door lock switch was announced molding), functional materials, and printing technolo-
using IME.[9,10] In general, the products that have gies. The integration of these technologies for the
reached the market represent simple manifestations of production of innovative products raises some technical-
the IME process. They are demonstrated in terms of pro- scientific issues, as interface requirements delineate their
totypes incorporating multiple LED, light guides, touch joint applicability.
switches or slides, etc.[11] These show the future develop-
ment direction.
In September 2019, TactoTek secured a license with 2.1 | In-mold labeling (IML) and in-mold
Korean LS Automotive, and along with a fellow license decoration (IMD)
with Faurecia, demonstrated the future direction for
HMI for automotive interiors.[3] Despite the technology The integrated decoration of polymeric parts can be done
not being relatively new, currently it is difficult to imple- by IML or IMD techniques (Figure 3). The main advan-
ment successfully, still requiring particular know-how tages of IMD/IML are the ability to provide functionality
and specific capabilities. The inherent technological chal- and increase the aesthetics of the product. IML and IMD
lenges are still being the focus of emerging solutions from refers both to the injection molding over a decorative
leading manufacturers. The main target market for this and/or functional film, their primary advantage being the
growing technology includes automotive, interiors and integration of several manufacturing steps, production,
exteriors, and white goods.[12] and decoration of molded parts into one operation.
The IME market is expected to show significant Therefore, by implementing these techniques, the need
growth from 2023/2024, starting from simpler products, for after-decoration is eliminated and final cost reduced.
consumer electronics and industries that can bring a Both techniques, although of similar basis, have dif-
product to market faster, for example, for the automotive ferent characteristics and are intended for different pur-
exterior. It will be developing toward more complex and poses. For instance, IML is used when there is a need to
higher-volume applications with more strict require- produce labels in injection molded products, i.e., its func-
ments, like overhead control units.[10,12] In addition, IME tion lies essentially in the information (marketing labels
products are expected to be seen in even more everyday that are cut pieces). In IML, the injection units are
devices, including household appliances and white goods, equipped with a robot whose function is to place a deco-
supporting the deployment of the internet of things, IoT, rative label in the appropriate location, which is fixed by
paradigm.[9] vacuum or electrostatic means. IML typically involves a
DuraTech Industries, Inc., which delivers custom small section of the injected part, usually characterized
label printing services, announced in 2019 its first com- by the absence of film in the corners of the piece.[14] On
mercial production of In-Mold Electronics (IME).[13] the other hand, IMD has a decorative function, the injec-
IDTechEx provides market research on emerging tech- tion is often done continuously using rollers (transfer
nologies, for instance in the field of printed and film) or a thermoformed film (film insert) that covers the
4 BELTRÃO ET AL.

full component. The ink transfer method requires, not PC, PC, PS, PE, PBT, PA6, and PA 66 were also used
only a specific kind of film, but also an appropriate ink. successfully.[16,17]
For instance, one of the most important ink characteris- As mentioned above, the polymer injection in the
tics must be high stretchability.[15] Typical applications IMD process can be over a thermoformed insert film.
include medical devices, consumer products, plastic This method has the most relevance for IME, since the
housings, automotive components, etc. IMD is often film is previously thermoformed and printed with con-
applied in the automotive industry, where the aesthetic ductive traces. The foil can also contain components such
aspect of parts inside the car is crucial. The surface finish as resistors, chips, or LED.[18] Despite the advantages pro-
can either have an aesthetic or protection function, or vided by the IMD method, there are some associated
even another type of purpose, such as to reduce the noise problems that affect the overall success of this technol-
level inside the car. In addition, it can hide superficial ogy. Due to unbalanced cooling enhanced by the decora-
defects or modify surface properties.[6] The main differ- tive film in IMD injection molding, part warpage can
ences between these techniques are presented in arise during cooling of the injected molded part, leading
Figure 4. to the development of residual stresses.[16,19] Several stud-
In both techniques, the film material needs to be ies have been carried out over time, for example, focused
chemically similar to the injected material in order to on evaluating the effect of the decorative film on mold
assurance a good bond and allow its recyclability. surface temperature during the molding process.[19,20]
The mostly used material is PP due to its general The results show that the IMD process introduces asym-
industry applicability, but materials such as ABS, ABS/ metric flow front advancement and uneven temperature
distribution in the mold core and cavity, leading to the
development of residual stresses and part warpage.

2.2 | In-mold electronics (IME)

In-mold electronics adopts IMD technologies based on


the category of molding with film insertion. They are
similar in the way they use thin printed films; however,
the functionality differentiates them. The IME process
creates a functional, visual, and human-machine inter-
face layer over a polymeric part. It combines the benefits
of the IMD process with functional electronics, by print-
ing conductive, semiconductor, and dielectric inks on a
polymeric film. The thin polymer printed foil can be ther-
FIGURE 3 Integrated decoration of injection molded parts moformed and then placed inside the mold where a

F I G U R E 4 Main
differences between IML and
IMD technologies
BELTRÃO ET AL. 5

F I G U R E 5 IME main processes


(adapted from “functional ink Systems
for in-Mold Electronics,” by DuPont)

polymer is back injection molded.[21] In this technique, printed conductive tracks are wide. For this reason, IC
the functional and graphic inks are printed on the flat requires wide pin pads, or narrow metallization tech-
film. The electronic components are then mounted using niques (thin linewidth printing techniques).[24,25]
conventional pick-and place equipment and SMD tech- Pick-and-place and SMD: In this technology, the
nologies that use low temperature processes (due to the electronic components are precisely placed by a pick-
used polymer substrate). The flat, functional film is then and-place machine. A conductive paste or conductive
3D formed before being back injection molded, as shown adhesives for surface mounting is usually dispensed. Typ-
in Figure 5. IME is a technology for structurally integrat- ically, SMD (surface-mount devices) are placed while the
ing electronic functionality into three-dimensional film is flat. The subsequently 3D thermoforming step
shaped parts.[22] The effectiveness of the IME process is shall not cause part damage, due to the process parame-
characterized by the selected materials. Therefore, con- ters. Using pick-and-place on an already-3D-shaped film
ductive inks have been developed to withstand elonga- requires special dispensing and pick-and-place machines
tion, adhesion to the substrates, and to support molding (higher degrees of freedom, DoF). Nowadays, conductive
and process conditions.[23] adhesives are the most used. However, very-low-
The interest of ink suppliers towards this technology temperature solders compatible with low-temperature sub-
has dramatically increased over the past few years, focus- strates can also be used.[26] More recently, liquid metals
ing especially on stretchable conductive inks. The IME is have been used as solder paste for mounting SMD and sen-
not a new process or technology, being an evolution of sors, due to their high stretchability and flexibility.[27]
IMD, in which molding (or other ways of 3D forming) Thermoforming: Subsequently, the foil is thermo-
are combined with graphic printing.[22] formed into a 3D shape, usually at high temperatures,
using vacuum or high air pressure (the applied values of
temperature, vacuum and air pressure are related to the
2.2.1 | IME process steps material to be thermoformed). The optimization of the
thermoforming process is crucial, and it must respect
The IME technology involves several steps as shown in the formability limitations of the functional materials.
Figure 6. The thickness of the film/foil (typically of 200–500 μm) is
Printing Flat Substrate: The process initiates with the an important parameter for the thermoforming process.
printing of functional inks, or stacks of functional mate- For instance, the design of electrical circuit patterns and
rials, on a 2D sheet. It is essential to control the printing the placement of electronic components where the least
and drying conditions, depending on the set and order of deformation is experienced is essential. It is required to
placement of materials used in the stack. Printing have stretchable printable functional inks that maintain
requires careful thickness control and proper adhesion their properties after the thermoforming step.
between the components, so that the designed electrical Trimming Connector: In this step, the film is trimmed
properties are maintained after the forming step. IC (inte- using part-specific die cutting tooling, thus facilitating its
grated circuits) packages have standard connectors placement inside the injection mold. Also, the connectors
designed for PCB applications (e.g., for surface mounted are mounted, providing the connection to the outside.[26]
technologies, SMT). In printed electronics, the screen- The connectors are assembled, usually using an
6 BELTRÃO ET AL.

FIGURE 6 IME process steps

anisotropic conductive adhesive or film (ACA or ACF), and substrate-molded polymer; ii) the integrated elec-
or by crimping. ACA/ACF allow the adhesive assembly trical circuit layout (circuitry and position of electronic
of connectors and other electronic components. They components) follows different rules from traditional
only conduct in the Z-axis (through-the-thickness) when PCB designs, and design guidelines shall be established;
placed between the printed electrodes and the connector/ iii) this design needs to consider the system function
component surface. The main advantages are related to and all the production processes (printing, mounting of
the low temperature and high interconnect density.[28] SMD, thermoforming, injection molding); iv) the
Injection molding: During injection molding, the design-to-production process is also not yet completely
printed film is vacuum or mechanically held in place and seamless.
the polymer is subsequently injected. In this step, high On the IME product use side, and depending upon
temperatures (170–320 C) and high pressure (of the order the specific sector requirements, the reliability of the
of 108 Pa) can be used. This stage requires optimization, functional molded parts needs to be validated and veri-
since the intrinsic variables of the process can cause the fied. For example, the requirements for an IME product
assembled electronic components to detach or cause the for a housing appliance are different from those of the
formation of air bubbles at polymer/printed substrate automotive sector. The strict requirements of polymeric
interface. Also, it is crucial that the CTE (coefficient of automotive components need to be fulfilled by the novel
thermal expansion) values of the materials are coherent, IME products. Furthermore, as polymeric materials are
thus avoiding potential deformations or detachments of being more often used in car interiors and exteriors,
the mounted electronic components.[26] where IME is being to have high applicability, this poses
The main challenges are (most of the time inter- additional challenges.[9]
connected): i) the inks shall have good electrical conduc- Finally, sustainability issues, including repairability
tivity/properties; ii) the ink and substrate need to be (life extension) and recyclability are of paramount impor-
compatible in terms of wettability, adhesion and print- tance. In fact, repair opportunities are limited or even not
ability; iii) the functional inks need to survive the for- possible. Given the embedded nature of IME products
ming and molding steps, being flexible, stretchable and separation and recovery of materials (ink, polymers) is
supporting flow, pressure and temperature conditions; iv) possible, but processes need to be established.[9]
mounting IC require adequate pads and positioning sup-
ports; v) the adhesives also need to support some elonga-
tion; vi) stacking materials for performing a given 2.2.2 | Applications
function is a huge challenge.
On the manufacturing side, a series of challenges can The first IME successful product, a thin and light overhead
be referred to: i) the printing processes shall allow console, was launched in a Ford car in 2012. As it became
smaller details; ii) new techniques for SMD are required more established, more suppliers of materials showed
to bonding electronic components over flexible organic interest, pushing it forward onto the market.[30] This tech-
substrates; iii) high throughput rates of functional films nology can be integrated into any application that includes
shall be available; iv) the development of knowledge and user interfaces, for instance control panels, electronics, and
tools for the optimization of thermoforming and injection appliances. Improvements such as LED, backlighting, and
molding is mandatory; v) lowering process cost processes EMI/RFI shielding, can be integrated into the designs.[30]
is demanding.[29] Many applications of this process use capacitive touch tech-
On the IME product design side, several challenges nology, which is an interface that replaces the tactile but-
can be identified: i) the choice of the pairs ink-substrate tons with the conductive touch of a human finger.[21] The
BELTRÃO ET AL. 7

ink traces are conductive and can include components properties, however, this can affect the electrical properties
such as resistors, chips, or LED. These run under the con- of functional inks.[4] Main types of inks for PE are conduc-
tact point and look for a change in the electrostatic field. tive, semiconductor, and dielectric inks/pastes.
The finger will act as a functional capacitor that attracts a Conductive materials: Electric conducting materials
charge to the point where it touches, activating a function. form the fundamental part of the electronic device layer,
IME technologies are achieving growing commercial defining the device structure and integrated circuit inter-
interest. Commercial development is currently in pro- connects. Typical conductive inks are based on metallic
gress in several companies, for instance TactoTek, which micro/nanoparticles. Among the metals used for printed
may be considered the market driver, as well as electronics, Ag based solutions are the most popular
Flexbright.[31,32] Other companies who have collaborated choice due to its good physical and electrical perfor-
in the development of IME solutions are Sun Chemical, mance on polymeric substrates.[36] In addition to silver,
Eastprint, DuraTech, AlSentis, and T + ink.[33] Dupont gold, platinum, copper, and nickel-based inks are also
provides printed electronics inks that tolerate severe pro- used. In this type of inks it is essential to avoid agglomer-
cess conditions while PolyIC and Kurtz are enforcing ation, promoting a proper dispersion of micro/
IME technologies to the automotive industry.[34] nanoparticles. Also, particle sizes are relevant for the
printing process. For instance, larger micrometric parti-
cles can be used in screen printing, but, on the contrary,
3 | DEVELOPMENTS ON I ME inkjet printing technology requires nanosized particles
CORE TECHNOLOGIES due to the small size of the nozzles. Besides, metallic
based inks show low deformation, thus fostering the
This section presents the developments on the several development of flexible and stretchable inks. Carbon/
components of printed electronics, such as inks, sub- Graphite nanomaterial-based inks are also available, all-
strates, printing and SMD techniques. In addition, the owing printing over large areas, good chemical stability,
constraints imposed by the thermoforming and over- mechanical flexibility, and lower costs. Despite the low
molding processes are presented for a full picture of cost and easy processing and improved stretchability,
recent developments of the IME technologies (Figure 7). organic conductors have much less electrical conductivity
than conventional metal-based inks (generally
include metal loadings of about 20–60 wt%).[37] Organic
3.1 | Materials for the IME process conductors are based on intrinsically conductive poly-
mers, such as poly(3,4-ethylenedioxythiophene)-poly
The IME process requires printable materials with spe- (styrenesulfonate) (PEDOT:PSS), polyaniline (PAN),
cific properties to allow appropriate printing of sub- polythiophene, polypyrrole (PPy), between others.[38]
strates. Typically, functional inks and pastes are to be Another range of electric conductive polymers developed
printed over substrates. for PE is founded on polymer nanocomposites made by
mixing conductive nanoparticles (e.g., metal, carbon
based) with elastomers, such as poly(dimethylsiloxane),
3.1.1 | Inks and pastes PDMS, and polyurethanes.[39]
Silver, gold, and copper nanoparticles inks are widely
The selection of an ink or paste with specific rheological used in PE for connecting elements in the electronic cir-
properties for the selected printing process is essential to cuits.[35] The world's leading manufacturers such as
develop a consistent printing process. The ink/paste viscos- Bayer, DuPont, and Sumitomo, are all fully involved in
ity shall be adequate to the selected printing process and the development of this technology.[40] The inks formula-
equipment. A variety of functional inks/pastes (organic and tions are highly formable and moldable based on 200 and
inorganic) have been explored for this purpose, such as 300% ink elongation. In general, the physicochemical
conductors, semiconductors, and dielectrics materials.[4] requirements for electrically conductive inks are identical
Most conductive inks are based on silver nanoparticles, to those for graphic or paint inks, but in addition they
since silver has the highest electrical conductivity among should provide good electrical conductivity of the printed
metals, in addition to being resistant to oxidation.[35] pattern. These inks should have compatibility with poly-
Ink viscosity is one of the main factors to consider in meric substrates and good processability during the print-
the printing process.[4] For instance, screen printing needs ing phase without affecting the electrical properties of
high viscous inks but, on the other hand, inkjet print tech- the final product.[35] Concerning the electrically conduc-
nology needs low viscous inks. Some ink formulations tive materials, the most common inks are based on con-
include additives to improve ink deposition and end-use ductive nano or micro particles components, which have
8 BELTRÃO ET AL.

FIGURE 7 Main technological steps for IME

been dispersed in a proper medium (water-based and sol- Organic semiconductor inks are mainly based on conductive
vent based inks). At present, most conductive inks are polymers. Frequently used organic semiconductors are poly
based on silver nanoparticles, since silver possesses the (3-hexylthiophene) (P3HT), poly(triarylamine), poly(2,5-bis
highest electrical conductivity among metals, being resis- (3-alkylthiophen-2-yl)thieno[3,2-b]-thiophene (PBTTT).[42]
tant to oxidation.[35] The required curing temperatures, Carbon nanotubes and graphene are also the center of stud-
typically in the range of 80–500 C, depend on the ink ies due to their high electron mobility.[43] Recently, emer-
composition, processing speed, and type of substrate. gent 2D nanomaterials, such as 2D allotropes of carbon
Recently several studies have been focused on printing (graphene), transition metal dichalcogenides (TMD) and
for patterning conductive features from metallic and Mxenes, have been used in semiconductor inks, allowing
carbon-based building blocks.[35] the fabrication of more complex devices.[44] Main relevant
Conductive inks can be thermal or UV cured. Ther- properties of semiconductor inks are electron mobility,
mal curing is commonly used in printed electronics, bandgap and other electronic properties. Although organic/
requiring high temperatures and long curing times. For inorganic semiconducting materials are used for printable
this reason, it is not suitable for large scale production electronics, inorganic semiconductors have greater proper-
and for all types of substrates.[37,41] Hence, a pulse ther- ties in terms of performance and stability, while organic
mal curing process has been introduced in the market, so materials have better flexibility and lower cost and the possi-
called photonic curing.[37] This is a thermal process that bility of processing at ambient conditions.
heats the ink/substrate by a pulsed light from a flash Dielectrics: For applications that require high capaci-
lamp. This allows keeping the substrate at relatively low tance in multi-layered printed assemblies, dielectric
temperature as it is heated only during a short time inter- layers are crucial for proper insulation to prevent leakage
val (c.a. 1 ms), being therefore a cure process suitable currents. Dielectric inks protect the circuitry and
for low-temperature substrates and R2R (roll-to-roll) enhance the operation of conductive materials. In most
manufacturing processes. On the other hand, UV curing PE, the semiconductor/dielectric interface is essential for
offers a more efficient and faster method, with low the right performance and the stability of the built device.
energy consumption. However, UV light hardly reaches A layer of dielectric material is necessary to promote the
the bottom of the printed pattern, which means that pos- activation of the medium caused by electric field or other
sible adhesion problems and non-uniform curing of large transduction phenomena.[4] Dielectric inks are usually
3D surfaces can occur.[41] Yet, UV-thermal dual-curing based on polymers, ceramics (e.g., zinc oxide, zinc and
technology has been presented to overcome the problems titanium dioxide, Ti02) and insulating 2D nanomaterials
associated with this type of curing.[37] (e.g., hexagonal boron nitride).[4] The most common
Semiconductor materials: Very few works have been dielectric materials in PE are poly(vinylpyrrolidone)
reported on inorganic semiconductors solutions and their (PVP), polystyrene (PS), poly(methyl methacrylate)
compatibility with printing techniques.[4] Inorganic based (PMMA), poly(vinyl alcohol) (PVA), poly(vinyl chloride)
semiconductor inks are typically based on metal oxides. (PVC), poly(vinylidene fluoride) (PVDF), and amorphous
Some inorganic semiconductors frequently used for this pur- fluoropolymers.[35] Also, epoxy resins have been used in
pose are Si, oxides of transition metals and chalcogenides.[4] some applications.[37] Polyurethane inks formulations
BELTRÃO ET AL. 9

TABLE 1 Main properties of some printable inks/pastes: Conductive, semiconductor, and dielectric[46–63]

Material Electrical conductivity (S m 1) Density (g cm 3) Elongation (%) Surface tension (mN m 1) Cost
Conductors
Ag 6.25  106-3.45  107 1.056 (5%) 42–60 42.16 (5%) €€
1.123 (15%) 45.29 (15%)
1.218 (25%) 46.65 (25%)
Cu 6.01  10 7
≈3.800 40 43–48 €€€
Ni 14.3  106 8.91 40 26–31 €€
Carbon-based 1.8  10 –25.0  10
3 3
1.100–1.240 72 30–35 €€
PEDOT:PSS 10–10 3
1.000 20–40 71 €
Liquid metals 3.4  10 4
6.080–6-360 30–50 624 €
Semiconductors
P3HT ≈105 1.040 20 29 €€
Mxenes ≈10 4
4.000 130 64 €
ZnO 10 –10
8 7
0.800 0.1 41 €
Graphene-based 0.08–4.1  10 4
0.933 20 32 €
Dielectric
PMMA - ≈1.000 1–3 24 €
PVA - 0.998–1.058 60–190 5–56 €
PVP - 1.001–1.029 5–50 42 €
PU - ≈1.050 >1800 42–48 €

have been optimized particularly for printing technolo- Metal foils and thin glasses are flexible substrates, but
gies.[45] These materials are all compatible with different not stretchable. The advancement of knowledge in mate-
printing or coating techniques. Besides being used as rials engineering has introduced stretchable electronic
dielectric layers in electronic devices, organic dielectric materials that can be bended, folded, rollable, stretched,
materials are also used for final encapsulation of printed and deformed. Printed electronics is influencing almost all
devices. Table 1 shows the main properties of printable manufacturing industries, being mechanically flexible sub-
inks/pastes. strates, such as polymers, providing new applications for
stretchable electronics.[65] Moreover, the flexibility of the
polymer substrates is the basis for low-cost high-speed
3.1.2 | Flexible substrates for IME manufacturing of devices using various printing tech-
niques. Printability, as the state of being printable, is an
The purpose of the final application and physical forms issue of polymeric materials, as they show low surface
of the substrates i.e., flatness, light weight, ruggedness, energies, typically, ranging from 0.025 and 0.04 J m 2.
conformability, foldability, stretch ability, are some of the Wettability characterizes the degree of wetting of a solid
features that affect their selection. Flexible substrates will surface by a liquid droplet, being evaluated by contact
also allow the adoption of continuous roll-to-roll angle measurements. Polymers are typically hydrophobic,
processing, eliminating the use of expensive and complex showing high contact angles (>90  C with water). Adhe-
processes (e.g., high vacuum and lithographic tech- sion is also a superficial phenomenon, depending upon
niques), promoting cost-effective mass production of interactions between the liquid ink and the surface of the
devices. Flexible substrates must have dimensional and substrate. Both wettability and adhesion result from inter-
thermal stability, low coefficient of thermal expansion molecular interactions and are important for a good print-
(CTE), excellent solvent resistance and good barrier prop- ability. The polymer substrate surface energy must be
erties for moisture and gases. Currently, there are differ- higher than the ink surface tension for proper wetting and
ent types of materials that could be used for flexible adhesion between the ink and the polymer substrate.[25]
electronic devices: metal foils, thin glass, and The major drawback in use of polymer substrates is
polymers.[42,64] their low glass transition temperature, Tg. Therefore, their
10 BELTRÃO ET AL.

FIGURE 8 Main polymers for flexible


substrates

maximum operating temperature is also low, typically are usually translucid. PEEK also presents a high sur-
<150 C, when compared to metal and ceramic substrates. face roughness and a high cost. Likewise, elastomers are
They also show low thermal stability. This limits their use becoming popular for this purpose, for instance silicone,
with some type of high temperature cure inks. In addition, being polydimethylsiloxane (PDMS) the most commonly
humidity has a major effect on the polymer material used used.[68]
for flexible substrates, affecting dimensional stability, and The main flexible substrates used in PE, as well as
the electric resistivity to a significant value. Polymers are their main physical properties are listed in Table 2. Some
divided into two main groups with respect to their morphol- important properties that the substrate must exhibit
ogy, semi-crystalline and amorphous, and into two main include thermal and mechanical stability, flexibility, sol-
groups with respect to their behavior when heated up, ther- vent resistance, surface roughness, surface energy, resis-
moplastics and thermosets (Figure 8). Their applications in tance to moisture, and barrier properties.
flexible electronics have been described elsewhere.[42] Semi-
crystalline polymers used in flexible electronics include
polyethylene terephthalate (PET) and heat stabilized PET, 3.2 | Printing techniques
polyethylene naphthalate (PEN) and heat stabilized PEN
and polyetheretherketone (PEEK). Amorphous polymer The possibilities of using different printing techniques
substrates include polycarbonate (PC), polyethersulfone have been extensively studied regarding the feasibility for
(PES), polyimide (PI), and polyetherimide (PEI).[42] Some of the manufacture of functional films. Selecting the suit-
these substrates are poor resistant to solvent absorption able printing process is essential to preserve the overall
compared to semi-crystalline polymers. compatibility of the printed layers and to ensure reliable
Beside these, several types of polymers have been pro- printed electronic structures. The relation between sur-
posed as flexible materials. Carbon nanotube (CNT) can face energy of the substrate and surface tension of the
be embedded in a flexible epoxy matrix as part of a fiber- ink is essential.[65] This means that ink, substrate selec-
reinforced polymer composite.[66] The development of a tion and printing process cannot be disassociated. The
piezoresistive strain sensor using an elastomeric compos- substrate must be selected according to the application
ite film made with polyurethane and CNT was demon- and printed ink. Likewise, ink selection must be associ-
strated. Another material that can also be used as a ated with the printing process and substrate compatibil-
substrate for printed electronics is paper.[66] ity. The selected printing process depends on the final
The most common substrates for IME are PET, PEN, product application and directly affects the printing reso-
and PC.[67,68] These polymer substrates are low cost, lution. The printing technologies can also be subdivided
optically transparent, with low surface energy, which in two main categories: contact and non-contact tech-
makes them suitable for PE. Polyimide (PI) is widely niques, as shown in Figure 9.
used in the commercial flexible PCB industry. However, In contact printing techniques, the patterned structures
it is expensive, has high surface roughness and the films with inked surfaces are in direct contact with the
BELTRÃO ET AL. 11

TABLE 2 Substrates for flexible hybrid electronics and their physical properties[66,69,70]

Young's Max. Surface


modulus deformation energy CTE
Substrate Transparency Density Tg ( C) (MPa) (mm mm 1) (mN m 1) (ppm  C 1)
PET 90 1.38 80 2.8 0.3–0.8 42–45 33
PEN 87 1.4 120–140 3.0–3.3 0.1 45 20
PI 35–60 1.42 410 2.5 0.90 57 8–20
PEEK 54 1.32 143 2.6–3.2 0.2–1.0 30–40 40–50
PLC (thermotropic) - 1.38–1.90 100–160 10–20 0.01–0.03 34–45 0–30
PDMS 92 0.97–1.03 125 0.6–4 0.6–1.3 19–24 300–400
Paper - 0.6–1.0 126–176 0.5–3.5 0.02–0.06 30–45 0.4–0.6

FIGURE 9 Printing technologies

substrate. On the other hand, in the non-contact technolo- methods. A squeegee is used to sweep the ink on top of the
gies, the ink solution is dispensed/sprayed onto the sub- screen with pressure, as the ink passes through the screen
strate from a very short distance. The printed structures and is transferred onto the substrate.[76] With this tech-
are defined by moving the substrate holder or ink dis- nique it is possible to get thick (>10 μm) features. How-
penser in a pre-programmed pattern. Some review articles ever, usually offers low resolution (c.a. 100 μm) and the
reported in this field are already available, for example, deposited film is rough due to the highly viscous (500–
focusing on inkjet printing, nanoimprinting, microcontact 5000 Pa s) nature of the inks/pastes used. Two different
printing techniques, and R2R fabrication.[71–74] The newly assemblies of screen printers can be used: flatbed and
developed polymeric stamp-based printing methods (soft rotary. In flatbed, the ink is squeezed across the screen
lithography), such as nanoimprint, micro-contact printing resulting in its transfer through the stencil openings to the
and transfer printing are of a growing interest.[4] Some of substrate below it. For continuous processing, a rotary
the techniques described below are already widely applied screen can be used (Figure 10).[4]
in the IME industry, while others have great potential to The print quality in screen printing is affected by
be gradually implemented. Some of the contact and non- numerous factors, such as the materials (ink and sub-
contact printing technologies are described below. strate), ink viscosity, printing speed, angle, geometry of the
Screen-printing: Screen-printing is the most developed squeegee and mesh size. The feasibility of this technique
and popular technology for PE since it has been the prac- for flexible electronics has been demonstrated through vari-
tice in the electronics industry for a long time (e.g., PCB ous printed sensors, electronics devices, and circuits.[4]
production). Furthermore, it is faster and more versatile in Despite all the advantages that this printing method has,
comparison to the other printing techniques.[75] Screen screen-printing also presents some challenges for the devel-
printing uses a porous mesh image carrier (screen), which opment of all layers of a flexible device.[77] For instance, it
produces thicker ink deposits compared to other printing produces large waste of production material (including
12 BELTRÃO ET AL.

ink) and the planar system speed is low in comparison to defined edges than gravure printing. With this technol-
other conventional printing processes.[25] ogy it is possible to obtain thin layers of about 1 μm, and
Gravure printing/gravure-offset printing: With this accomplish patterns with resolution of 20 μm.[4] The
technique, it is possible to produce high-resolution pat- dynamic viscosity of ink is usually between 0.05 and
terns at high speeds. It can achieve feature printed sizes 0.5 Pa s. Flexographic printing is susceptible to film insta-
of a few μm (<20 μm). The features are engraved in the bility, which promotes many defects such as open lines,
cylinder, which are filed with ink. A doctor blade wipes overlapped lines, and edge waviness effects.
the excess ink from the cylinder (Wiping). Then, the Microcontact printing is a soft lithography technique.
cylinder rolls over the substrate and the ink are trans- μCP is based on the conformal contact of patterned elas-
ferred onto it (Transfer), creating the final pattern tomeric stamps with a target surface, in which proper
(Figure 11).[78] Once the substrate is wetted, ink spreads control of the stamps on micrometer scale is required.
over it forming the final printed pattern (Spreading). For This technique makes it possible to produce multiple cop-
large-area and high-volume manufacturing, gravure ies of 2D patterns using a patterned stamp developed
printing is the great choice. It is capable of producing through a master mold.[82] The stamp is typically made
high quality and cost-effective patterns, typical of an R2R from PDMS, which is the elastomer often used due to its
process. The printed films have a broad thickness range, properties, such as conformability to large areas, elastic-
typically 1 to 8 μm. Solution properties and cell width/ ity for easy release, low surface free energy, chemical
depth ratio have significant importance in gravure print- inertness, homogeneous, isotropic, optically transparent
ing along with other system parameters.[79] The low vis- and durability.[82] Review of the evolution, addressing
cosity inks (dynamic viscosity of ink between 0.05 to the new variations and applications of μCP over the past
0.2 Pa s) allow emptying of the cells and achieving better
line resolution.[4]
Gravure-offset printing is a developed version from
gravure printing, in which a blanket is used to prevent
damage to the cylinder due to direct contact with the sub-
strate.[80] The printed pattern is defined by differences in
wetting of a plane surface. The elastic blanket collects the
ink from the grooves of the cylinder and transfers it to
the desired surface. Several process parameters affect the
printing results, although the dependence on the printing
speed and blanket's thickness is of great importance due
to the minimal contact time between ink and the blan-
ket.[81] It is possible to obtain high resolution (<20 μm)
and thin layers down to 0.5 μm.
Flexographic printing: Flexographic printing is applied
for high-speed runs of PE.[80] Various inks can be used
for this technique with a rubber or polymer plate having
patterns, developed by photolithography, and attached to
a cylinder (Figure 12). In contact with the inked areas of
the anilox cylinder, the patterns on the plate cylinder
serve to print on the substrate that passes between them.
This method offers better pattern reliability and better- FIGURE 11 Illustration of gravure printing technique

F I G U R E 1 0 Illustration of screen-
printing process
BELTRÃO ET AL. 13

F I G U R E 1 2 Illustration of
flexographic printing

few years are discussed in detail elsewhere.[83] Some chal- Nano-imprinting (NI) lithography: Nano-imprinting is
lenges associated with μCP printing include the diffusion another soft lithography technique. NI is used to pattern
of self-assembled monolayers (SAM) areas not contacted materials by mechanical and physical deformation of a
by the stamp, the broadening of features, and the blur- wet layer, using a hard or a soft mold with nanoscale pat-
ring of the feature edges. This technique requires precise terned structures on the surface (Figure 14). The mold is
adjustment of the surface energies for efficient ink trans- pressed to form a solution on a substrate, at a controlled
fer, either by chemical modifications or topography, from temperature and pressure, creating a thickness contrast
mold to the substrates.[73] into the layer. A thin residual layer of polymeric material
Lithography: Lithography is the process of transfer- is left underneath the mold flanges, acting as a soft soft-
ring patterns from one medium to another. This ening layer that prevents direct impact of the mold on
method relies on the action of two wetting functions on the substrate, effectively protecting the nanoscale fea-
the surface of a flat and unbossed printing plate tures of its surface.[87] The interface and surface charac-
(Figure 13).[84] The ink is moved to an intermediate car- teristics have a big influence on the demolding capability
rier or “blanket,” which transfers the image to the sub- and filling behavior, influencing the final pattern qual-
strate. The plate has image areas that are hydrophobic ity.[88] In addition, it is essential to have a controlled pres-
(ink accepting/water repelling) and non-image areas sure in order not to destroy the printing patterns.[88]
which are hydrophilic (water accepting/ink repel- Several NI approaches are being developed, for example,
ling).[85] The non-image areas are covered with a solu- thermal, photo, ultraviolet (UV), step-and-flash, and
tion, normally composed of water with additives to roller nanoimprinting.[4] The critical challenges for NI
lower its surface tension, helping to obtain a more com- include overlay alignment, template fabrication, defect
plete wetting of the non-image areas of the printing control, and high yield.[89]
plate. The ink is applied to the image areas of the plate, Furthermore, some of the most used non-contact
by means of distribution rollers, ensuring constant film printing technologies are described below.
thickness.[85] The mutual repulsion between ink and Inkjet printing: Inkjet printing is a digital printing pro-
water keeps the non-image areas without ink. The ink cess, heavily used for prototyping and large-volume
only transfers from the image areas of the plate. The manufacturing of electronics.[78] Typically, the ink reser-
ink is transferred from the printing plate to a rubber voirs of inkjet printers are coupled with piezo constrictors
covered cylinder (blanket), and then printed on the sub- that load and expel ink. In this process, each droplet can
strate.[85] The resolution limit of the process is between be controlled, so the ink consumption is very low. Thick-
0.1 and 0.01 mm.[84] Offset provides very high print ness about 100 nm can be achieved, however, with moder-
quality and is commercially attractive for a wide range ate resolution (c.a., 50 μm). The dynamic viscosity of the
of run lengths. Waterless lithography is an alternative ink is usually 1 to 20 mPa s. Semiconducting, insulating,
way of printing that uses a silicone rubber layer on the and metallic low viscosity inks can be printed with inkjet
plate surface to repel ink in the non-image area.[86] printing.[90] The printed patterns are digitally generated
14 BELTRÃO ET AL.

F I G U R E 1 3 Illustration of
the lithography process

FIGURE 14 Representation of different nanoimprinting techniques


BELTRÃO ET AL. 15

F I G U R E 1 5 Inkjet printing
methods: Schematics of (A) CIJ,
and DOD inkjet printing with
(B) piezoelectric, and
(C) thermal head

(CAD software) and can be easily changed, which makes resolution and independence of orientation. AJP provides
this printing technique an ideal choice for prototyping. consistent deposition at nozzle–substrate offsets of
Resistors, capacitors, and inductors are developed using 1–5 mm.[93]
inkjet printing on polyimide substrate with various func- Slot-die printing: During this printing method, a
tional inks.[4] A disadvantage of inkjet is that it consists of liquid is pumped from a reservoir through a thin
a raster motion for printing, which makes the printing slot and deposited onto a substrate (Figure 17). It is
process slower compared to roll-to-roll processes. Inkjet in becoming a preferred process due to its low operational
comparison to flexography and gravure printing processes cost and potential to be used in large-scale mass
results in rougher and less uniform ink morphologies.[91] manufacturing.[95]
Chemical stability, solvents solubility and low temperature In addition, slot-die printing is capable of achieving
processing are some of the key requirements of inkjet extremely uniform films across large areas. This method
printable materials. allows the film thickness to be predetermined by con-
In inkjet printing, there are two basic types of print- trolled parameters. It is applicable for solutions with a
heads: Continuous Inkjet (CIJ) heads and Drop-on- wide range of viscosities and processing speeds up to
Demand (DOD) heads. As shown in Figure 15A), CIJ is a 200 m/min.[95] One of the main advantages of this tech-
method where a stream of ink droplets is continuously pro- nique over traditional ones is that it can easily be inte-
duced and jetted. The droplets are charged by the electrode grated into scale-up processes, including R2R.
and subjected to an electrostatic field, being deflected to Laser direct writing (LDW): In laser direct writing
deposit on the substrate.[92] On the other hand, in the technique, a pulsed laser is used to induce the transfer of
DOD method, the ink droplets are only generated when material from a source film onto a substrate. The laser
required, through a piezoelectric or a thermal inkjet pro- pulses spread through the transparent substrate, being
cess (Figure 15B,C). CIJ method allows a higher printing absorbed by the film.[96] The movement of the source,
efficiency. However, the complexities inherent in jet con- and receiving substrate, enables the 3D pattern forma-
trol, diversion and recycling of the inks have limited the tion. The galvanometric scanning mirrors enable rapid
application of this technique. Therefore, DOD has devel- motion and high-resolution patterns from the written 3D
oped as the main inkjet printing technology.[92] volumetric pixels (voxels). LDW manages the deposition
Aerosol jet printing: In this method, the functional ink and transfer of complex materials for which it is essential
is aerosolized and entrained in a gas stream (Figure 16). to maintain the physical, biological, and/or chemical
The system can use two options to generate the aerosol properties in the patterns.[96] Materials such as organic
from inks with viscosities between 1 to 1000 mPa s: ultra- and biological molecules are particularly vulnerable,
sonic or pneumatic.[93] The aerosol stream is directed to a where the transfer mechanism can cause damage in these
print head where it is aerodynamically focused by a coax- systems.[97]
ial sheath gas flow.[94] The free-form deposition coupled Roll to roll (R2R) printing techniques are character-
with a relatively large stand-off distance of the aerosol jet ized by being a continuous and high throughput process
printing (AJP) technique, enables the production of for deposition of various materials on large substrate
devices with increased geometric complexity compared to rolls. A R2R line is equipped with several rollers on
other printing techniques.[93] This technique has a wide which the web (flexible substrates) passes with controlled
material compatibility, being suitable for printing con- tension.[98] Processing sections on a typical R2R line
ductors, semiconductors, and dielectrics. It has a high include tools for deposition, patterning, lamination, and
16 BELTRÃO ET AL.

F I G U R E 1 6 Illustration of aerosol
jet printing process

3.3 | Developments on IME

As above-mentioned, several semi-crystalline and amor-


phous polymers have been suggested as flexible substrates
(e.g., polycarbonate, polyimide, polyethylene naphthalate,
polyethylene terephthalate, PVDF).[110–113] Also, some flexi-
ble substrates (e.g., poly (PDMS), polyurethane, thermoplas-
tic polyurethanes). [25,111,114,115] The mechanical properties
of a range of commercial IMD films (PC, blends of PC with
PBT and PET) were evaluated in order to understand their
performance and suitability over the full range of tempera-
tures and pressures used in the IMD process.[116] The
mechanical behavior of the polymeric films and their tem-
perature response are related to the polymer molecular
structure, as would be expected. PC is an amorphous poly-
mer, so due to the random arrangement of molecules its
mechanical behavior does not vary depending on the direc-
FIGURE 17 Illustration of the slot-die printing process
tion of deformation. On the other hand, crystalline poly-
mers (e.g., PBT) have a more orderly structure, and the
packaging based on the structural requirements of the elastic modulus and yield stress increase with the degree of
device.[4] Gravure, offset, flexography, rotary screen crystallinity.[117,118]
printing and nanoimprint techniques are some of the Since the properties and deformation of polymeric
favorable methods for R2R configuration.[80] R2R fabrica- films are significantly affected by the behavior of the
tion is more suitable for organic or polymer based thin injected polymer, it was numerically investigated the
film devices, it has been also explored for solar cells, light deformation of the polymer film and the injected poly-
emitting diodes, and display devices.[99] Recently, it has mer during the IMD process.[119] The injected molten
been reported the combination of slot-die coating and polymer could lead to tearing of the polymer film in the
laser direct writing on a R2R setup for development of regions near the corners. The mold temperature is con-
piezoresistive strain sensors.[100] One of the main chal- sidered a critical parameter for the IMD process, since
lenges of this fabrication method is how to model the the ink behavior is affected by the temperature. To
combined effects of material, structure, and process, opti- investigate the effect of temperature on the film, Shia-
mizing them to create multi-layered flexible sensors and Chung Chen et al.[120] injection molded PC under sev-
devices with desired performance.[80] eral conditions, including mold and melt temperatures,
As the selection of printing technique depends on ink film material, and thickness. It was found that with the
properties and printed feature requirements, a comparison increase in film thickness, the difference in mold tem-
of the different printing techniques is provided in Table 3, perature induced by the heat retardation, caused by the
listing ink and printed feature properties. film, also increases.
BELTRÃO ET AL.

TABLE 3 Comparison of several printing techniques[3,4,25,93,95,101–109]

Contact printing technologies Non-contact printing technologies

Screen- Gravure/ Nano- Laser direct


printing Flexography gravure-offset imprinting Lithography Aerosol jet writing Slot-die Inkjet
Image Carrier Stencil Relief Engraved Polymer stamp Flat Plate Jet Pulsed laser Doctor blade Digital
Resolution (μm) 30–100 30–80 50–200 ≈1 20–50 20 <0.1 200 15–100
Printing area Medium Large Large Medium Large Large Medium Large Large
Printed layer thickness (μm) 3–30 0.17–8 0.02–12 0.01–0.03 0.6–20 0.01–5 0.056 0.15–60 0.01–0.5
Printing speed (m/min) 0.6–100 5–180 8–100 0.006–0.6 0.6–15 0.3–0.6 1200 0.6–5 150
Ink viscosity (Pa s) 0.5–50 0.01–0.5 0.1–1 0.10 0.1–10 0.0007–5 0.014–10 0.1 0.01–0.02
Solution surface 38–47 13.9–23 41–44 22–80 22–80 30 - 65–70 15–25
tension (mN m 1)
Material wastage Yes Yes Yes Yes Yes No No Yes No
Cost Low Low High Low High Low Medium Low Low
Design Flexibility High Low Low High High High High High High
Substrate Any kind Polymer, Polymer, Paper, Polymer, Polymer, Polymer, Polymer, Glass, Polymer, Any kind
Paper, Board Flexible Silicon, Glass Paper, Board Silicon, Glass Metal, Ceramic Flexible
substrates substrates
17
18 BELTRÃO ET AL.

Film thickness was found to influence the deforma- after the thermoforming process. [127] The LEDs joints
tion conditions, specifically under plane stress and plane showed good structural integrity.
strain conditions. The same study demonstrated that the A recent report discussed the prediction of ink-wash
modulus of elasticity value decreases when the specimen and part warpage based on the molding parameters.[128]
thickness increases.[121] Earlier works acknowledge that Ink wash-off is caused by the high shear stress between
thicker specimens present greater stiffness, and a reduced the stationery ink/film and the flowing polymer melt.
capacity of the sample to deform in the transverse direc- The chance of the ink to be removed from the film
tion.[122] Film thickness affects the cooling rate in the increases, if the shear stress is higher than the adhesion
injected melt polymer, as a consequence, it affects the between the ink and the film. Ink wash-off has been one
solid-state characteristics of the part. Mold wall thickness of the problems that interfere with the success of the
is extremely important, especially near the gates. Thin IMD process for injection molded parts. This can be
walls near the gates cause extreme shear stress on the avoided by protecting the printed pattern with an overlay
inks.[123] In a report, after examining the effect of the dec- (lamination), but this will make the film thicker. An
oration film on the mold surface temperature during the experimental matrix design based on the Taguchi method
injection molding process, it was found that, when was carried out to investigate the influence of processing
the film thickness increases, the retardation induced by parameters on the ink wash-off of molded parts.[123] In
the mold temperature difference also increases. PC and this study, samples of three different thicknesses were
PEI films were studied, with thickness ranging from molded. The experimental results showed that molded
0.1–2 mm.[120] The modulus of elasticity values decreased parts of smaller thicknesses exhibited more severe ink
when the specimen thickness increased.[121] wash-off. The melt and mold temperatures were the main
The interfacial characteristics of PC/ABS and PET factors affecting the ink failure of IMD injection molded
films were explored, and it was concluded that the adhe- parts. Also, the ink was mainly washed off by the high
sion between the film and the PC/ABS substrate shear stresses applied from the hot polymer melts.
is influenced by the molecular weight of PC and Throughout the study, it was concluded that most of the
PC-oligomer in the blends.[124] On the other hand, in ink wash-off occurs near the gate, gradually decreasing
PET films, it was due to the molecular orientation and as the distance from the gate increases. In addition, it
crystallization processes. It was also investigated the was established that IMD molded parts of smaller thick-
effects of the process parameters of PC film for IMD, after nesses showed more severe ink wash-off than those of
examining the effect of decoration film on mold surface greater thicknesses. The polymer films are subjected to
temperature during the molding process.[117] At an opti- both shear and elongational stresses during this process.
mized temperature, the formability of the film was dem- As the injected polymer starts to solidify, as soon as it
onstrated to be limited to very smooth contours. The touches the walls of the mold, a highly oriented skin
prototypes that exhibited the least amount of light scat- layer is produced. The consequent elongation of the plas-
tering and, therefore the least amount of print-through, tic film can result in the delamination of the printed inks.
exhibited certain undesirable irregularities by industry The combined effects of high shear stress and high melt
standards. These irregularities can be attributed to several temperature resulting from the process may lead to the
causes, such as mold surface finish.[117] wash-off of the ink from the decoration films. Through
A few studies have been carried out concerning the fea- the experimental results, it was recognized that the incre-
sibility of the IMD process and the consequent ability of ink ment upon the melt injection pressure helps to minimize
adhesion on polymeric substrates.[125] Adhesion and the ink wash-off in IMD molded parts. In addition, the
stretchability of silver inks printed on stretchable substrates, wall thickness near the gate is extremely important, as
like PDMS, to form conductive patterns have been investi- thin walls near the gate cause high shear stresses on the
gated for stretchable electronics applications.[126] Stretch- inks, resulting in damage to the part.
able conductive polymers, which can be deformed and The effects of production parameters on the viability
extended to a certain level of strain at high temperature, of PC film for IMD in resin infused composite compo-
allow the standard manufacturing process for polymers, nents were investigated.[123] The statistical validation
such as thermoforming, to be implemented in electronic indicated minimal print-through at a forming tempera-
applications.[127] The temperature of the mold surface is the ture of 147 C. The increase of the mold temperature cau-
most important process parameter for an ideal ink transfer ses a decrease on the ink wash-off. However, a too high
to the polymer. A study focused on the effect of the combi- mold temperature keeps the temperature of the poly-
nation of printing in surface mount technology and the- meric material warm for a long time, which, in turn, can
rmoforming concluded that the part (PC substrate with lead to wash-off of the inks.[123] Also, most of the ink
printed conductive ink) exhibited good physical conditions wash-off appears near the gate and gradually reduces as
BELTRÃO ET AL. 19

the distance from the gate increases. IMD molded parts uneven temperature distribution in the mold core and
of smaller thicknesses exhibit more accentuated ink cavity, leading to residual stresses and warpage of
wash-off than those of bigger thicknesses. This can be parts.[120] More recently, it was examined the warpage of
explained by the fact that injection molded parts have a IML injection molded components and established that
higher shear stress near the gate during filling. Through it is the volume shrinkage difference between the label
an experimental test, it was recognized that the incre- and substrate that causes bending in the parts in the
ment upon the melt injection pressure helps minimize opposite side of the label.[132] The warpage decreases as
the ink wash-off in IMD molded parts.[123] the injection velocity increases. Therefore, they proposed
The manufacturing of MID via IMD technology has that this problem can be dealt with by varying the tem-
been investigated.[40] Printing ink mixed with several peratures of the mold. Also, it was investigated, both
conductive materials was studied for electrical conductiv- experimentally and numerically, the warpage in IMD
ity after printing on a thin film. Carbon black was found injection molded parts, concluding that all molded parts
to have a better electrical conductivity and a lower cost warped toward the side of the decoration film. In the
than other materials. During the injection of the polymer, experiments, the corner angle of the molded parts and
no wash-out of the conductive ink printed on the film the injection pressure of the molten material, were the
surface was observed. The tested PC film was compatible main factors that affect the warping of IMD injection
with the PC/ABS blend substrate, and no film peeling molded parts.[19]
was observed. Several studies are focusing on the production of elec-
The IME molding process can introduce asymmetric tronic products with functional circuits printed on flexi-
frontal flow advancement and uneven temperature distribu- ble foils instead of conventional rigid PCB. The capability
tion during the injection molding step due to the presence of integrating electronic functions into the final parts
of the inserted polymeric film, which can result in the brings improvement of functions and enhancement of
development of residual stresses and part warpage. Until quality in various industries, such as the automotive sec-
now, several studies were made to examine the warpage of tor. Production of functional electronic devices based on
IMD injection molded parts. Chiang et al.[129] investigated flexible substrates can result in a cheaper and more effi-
the warpage in thin wall parts replacing insert molding cient manufacturing solution in comparison with con-
with thin-wall injection molding to fabricate electronic dic- ventional batch processes used nowadays.[33] The
tionary battery covers. They concluded that melt tempera- potential of IME technology has been verified by VTT in
ture is the most important process parameter for warpage photonic over-molded flexible foil structures, over-
during thin-wall injection molding. Also, low melt tempera- molded optical touch panels, over-molded semiconductor
ture, high injection velocity, and high packing pressure electronics and LED lighting.[133] Recently, it was built
eliminate part warpage during thin-wall injection molding. an intelligent system combining printed and flexible
An investigation on process modeling and simulation was components, including an electrochromic (EC) display
also previously made.[130] A simulation software was devel- component that was integrated into and injection molded
oped with modules of stress and warpage analyses. The 3D component to create a final product.[134] The feasibil-
comparison between simulation and real product indicates ity of thermoforming electronics incorporated in a ther-
that the developed code, could be effective to the prediction moplastic matrix has also been shown.[1] The results are
of part warpage.[130] For a PC film, it was found that the promising and indicative of the robustness of the elec-
heat transfer retardation results in a mold temperature drop tronic systems. However, it was also shown that the
in cavity surface and the maximum temperature drop, as direct dependence between the deformation and the film
compared to that of conventional injection molding without thickness is still a limitation of the process.[135] TactoTek
film, may be as high as 17.7 C. For PET film, the maximum has demonstrated IMSE (in-mold structural electronic)
mold temperature drop is about 13 C.[120] parts with 70% weight and 90% thickness reduction,
Baek et al.[131] studied the effect of the processing when compared with conventional assemblies.[1]
conditions on the warpage of the IMD injection molded To form a 3D electronic device, it was explored the
parts. They concluded that the warpage decreases as the effect of combining the standard printing process and the
injection velocity increases. Through simulation results, thermoforming process in a stretchable conductive poly-
it has been shown that greater warpage occurs in regions mer. The results showed good performances of LED
with higher stable temperatures, after demolding the joints, and the stretchable conductive polymer showed
part. In a report, after examining the effect of the decora- good physical conditions after thermoforming. It
tion film on the mold surface temperature during the exhibited minor voids in the corner of the product after
injection molding process, it was found that the IMD thermoforming, which do not significantly affect the
process introduced asymmetric flow front advancement, lighting of the LED.[127]
20 BELTRÃO ET AL.

TABLE 4 Acknowledgements of the different variables of IMD process

Variables Causes/problems Acknowledgments


Thickness • Influences the deformation conditions, namely the • The modulus of elasticity values decrease when the
plane-stress and plane-strain;[121] specimen thickness increases;[121]
• Thin walls near the gates cause extreme shear stress • The influence of thickness on Kc has been studied in
on the inks;[123] HIPS and in PC. Plane-strain fracture was found above
• Thicker specimens present greater stiffness, but lower 40 mm thickness and Kc was constant.[121]
deformation capacity in the transverse direction.[121]
Ink wash-off • The injected molten polymer could lead to tearing of • On a PC film at 160 C, the forming capability was
the polymer film in the regions near the corners;[119] maximized, and the surface finishes exhibited high
• Ink wash-off is caused by high shear stresses between print-through;[117]
the stationery ink/film and the flowing polymer • Satisfactory results (no ink wash-off) were achieved
melt;[128] between 80 C and 100 C of mold wall temperature;[125]
• Part thickness, mold and melt temperatures are the • In PET films for IMD, it was established a processing
most significant factors affecting the ink wash-off;[123] window with a temperature range of 200–220 C and a
• An increase of injection velocity increases the ink stretching speed of about 500 mm min 1;[136]
wash-off radius;[128] • For a PC film, statistical validation indicated a minimal
• Most of the ink wash-off appears near the gate and print-through at a forming temperature of 147 C;[123]
gradually reduces as the distance from the gate • The increment upon the melt injection pressure helps
increases;[123] minimize the ink wash-off in IMD parts.[123]
• IMD parts of smaller thicknesses exhibit more
accentuated ink wash-off than those of bigger
thicknesses.[123]
Warpage • Melt temperature is the most important process • For a PC film, the heat transfer retardation results in
parameter to avoid part warpage during thin-wall the mold temperature drop in the cavity surface, and
injection molding;[129] the maximum temperature drop, may be as high as
• Greater warpage occurs in regions with higher stable 17.7 C. For PET film, the maximum mold temperature
temperatures, after demolding the part;[130] drop is about 13 C.[120]
• The warpage decreases as the injection velocity
increases;[131]
• All molded parts warp toward the side of the
decoration film.[19]

IME allows the integration of electronics functions/ 4 | CONCLUDING REMARKS


components on the inner surface of injection molded
components during their molding steps. Recently, other In-mold electronics technology has gained relevance for
alternative technologies have also emerged that create applications in several industries over the past years.
the electric circuitry and perform the insertion of elec- Recent reports predict that this technology will continue
tronic components after the injection molding process, to show great growth over the next 10 years. IME is an
such as 3D molded interconnected devices (3D-MID) emerging global trend towards 3D structural electronics,
with laser direct structuring (LDS), 3D printing and 3D associated with a departure from the already rudimen-
surface mounting technologies. These technologies allow tary practice of encasing components (e.g., PCB) inside
mounting the electronic functions/components in both a polymeric box. There are still some drawbacks associ-
the outer and inner side of the injection molded part, not ated with this technology, however the inherent promis-
requiring them to withstand the high temperatures, pres- ing advantages are appealing to several industrial
sures, and deformations of the IMD process. Both IME sectors.
and non-IME technologies have not yet been compared IME technology has been the target of several studies
in terms of costs, company logistics and economical and innovations over the last years, and some technologi-
added-value (e.g., supply chain management, financial cal issues have been already addressed. The interactions
investment analysis, intellectual properties rights, inter- between ink and substrate, the thermoforming step of the
nal technology know-how). printed film and its overmolding by an injected hot poly-
In Table 4 is presented a summary of the several stud- mer are strong. The processing conditions (temperatures,
ies, and resulting conclusions, for the IMD process pressures, flow rates) of this later step are of paramount
variables. effect. The insertion of a thin film, typically of few
BELTRÃO ET AL. 21

hundreds of micrometers, in the injection mold cavity and UIDP/05256/2020, financed by FCT—Fundaç~ao para a
has been proved to create an asymmetric frontal flow Ciência e Tecnologia, Portugal.
advancement and an uneven temperature distribution,
resulting in the formation of residual stresses and part CONFLICT OF INTEREST
warpage. The thickness of this film influences its defor- The authors declare no conflict of interest.
mation conditions (namely under plane stress or plane
strain conditions) and capabilities. Also, with the incre- ORCID
ment of the film thickness, the difference in mold tem- Júlio C. Viana https://orcid.org/0000-0002-1210-2915
perature also increases, as this film acts as a thermal
barrier for cooling. Furthermore, the inserted polymeric RE FER EN CES
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27, 224. mer Engineering at the University of
[124] Y. W. Leong, M. Kotaki, H. Hamada, J. Appl. Polym. Sci. Minho. He graduated in Industrial
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a PhD in Science and Polymer Engi-
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neering from University of Minho in 2003. He
[127] M. F. M. Sharif, A. A. Saad, M. K. Abdullah, N. A. Aziz, N. A. develops research activities at the Institute of Poly-
Ismail, F. C. Ani, M. Y. T. Ali, Z. Samsudin, IEEE, New York, mers and Composites Research Unit, IPC, in the-
U.S. 2018 IEEE 38th Int. Electron. Manuf. Technol. Conf. rmoforming, fused filament fabrication, FFF, and in
IEMT, https://doi.org/10.1109/IEMT.2018.8511656. the development and characterization of degradable,
[128] S. P. Sun, T. H. Su, D. Hsu, Presented at Annu. Tech. Conf.— biodegradable polymer materials.
ANTEC, Conf. Proc., Anaheim, Society of Plastics Engineers,
Connecticut, U. S. 2017. Júlio C. Viana received its PhD in
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[130] F. Liu, H. Zhou, D. Li, J. Reinf, Plast. Compos. 2009, 28, 571. Minho in 2000, a MSc. in Computer
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[133] T. Kololuoma, M. Keränen, T. Kurkela, T. Happonen, M. Belfast, UK, in 1993, and Graduated
Korkalainen, M. Kehusmaa, L. Gomes, A. Branco, S. Ihme, in Industrial Engineering—Plastics Branch, Univer-
C. Pinheiro, I. Kaisto, A. Colley, K. Ronka, IEEE J. Electron sity of Minho in 1991. He joined University of Minho
Dev. Soc. 2019, 7, 761. as professor in 1991, being currently Associate Profes-
[134] T. Kololuoma, M. KerÄnen, T. Kurkela, T. Happonen, M. sor, at the Department of Polymer Engineering, Uni-
Korkalainen, M. Kehusmaa, L. Gomes, A. Branco, S. Ihme, versity of Minho. He is currently the director of IPC—
C. Pinheiro, I. Kaisto, A. Colley, K. Rönkä, IEEE J. Electron
Institute for Polymers and Composites, a research unit
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[135] C. Kallmayer, F. Schaller, T. Loher, J. Haberland, F. Kayatz,
from U. Minho.
A. Schult, IEEE, New York, U.S. 2018 13th Int. Congr. Molded Vitor Paulo received its MSc. in
Interconnect Devices. https://doi.org/10.1109/ICMID.2018.
Mechanical Engineering—Design
8526929.
and Product Development from Uni-
[136] M. Amran, S. Salmah, M. Zaki, R. Izamshah, M. Hadzley, S.
Subramonian, M. Shahir, M. Amri, Adv. Mater. Res. 2013, versity of Aveiro in 2010 and Gradu-
903, 61. ated in Mechanic Engineering—
Production, IPLeiria in 2004. He is
currently the Chief Technology Inno-
vation Officer at GLN and previously was the Head of
AUTHOR BIOGRAPHIES Operations at the GLN Plastics Unit since 2018. He
has experience in the plastics production and the
Mariana Beltr~ ao received its MSc. implementation of automated production lines since
in Polymer Engineering from Minho 2000. It also has a high know-how of technology and
University, Portugal, in 2018. Cur- tools for injection processes, as well as the manage-
rently, she is a researcher in IPC— ment and coordination of Innovation projects.
Institute for Polymers and Compos-
ites, hosted by the Polymer Engineer-
ing Department at Minho University.
Her work focuses on In-Mold Decoration (IMD) with How to cite this article: M. Beltr~ao, F.
printed decorative and functional films (i.e., In-Mold M. Duarte, J. C. Viana, V. Paulo, Polym. Eng. Sci.
Electronics (IME)). 2022, 1. https://doi.org/10.1002/pen.25918

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