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Japanese Journal of Applied Physics 61, SE0803 (2022) PROGRESS REVIEW
https://doi.org/10.35848/1347-4065/ac621a

Advancing flexible electronics and additive manufacturing

Alejandro H. Espera Jr.1,2 , John Ryan C. Dizon3, Arnaldo D. Valino4, and Rigoberto C. Advincula5,6,7*
1
Electronics Engineering Department, School of Engineering and Architecture, Ateneo de Davao University, Davao City, 8016, The Philippines
2
Department of Engineering Education, College of Engineering, Virginia Polytechnic Institute and State University, Blacksburg, VA 24061, United States
of America
3
Design, Research and Extension in Additive Manufacturing, Advanced Materials and Advanced Manufacturing (DR3AM) Center/Industrial Engineering
Department, Bataan Peninsula State University, City of Balanga, Bataan 2100, The Philippines
4
Mechanical Engineering Department, College of Engineering, Adamson University, Manila 1000, The Philippines
5
Department of Macromolecular Science and Engineering, School of Engineering, Case Western Reserve University, Cleveland, OH 44106, United
States of America,
6
Department of Chemical and Biomolecular Engineering and Joint Institute for Advanced Materials, University of Tennessee, Knoxville, TN 37996 United
States of America
7
Oak Ridge National Laboratory, Center for Nanophase Materials and Sciences, Oak Ridge, TN 37830 United States of America
*
E-mail: [email protected]
Received December 7, 2021; revised March 14, 2022; accepted March 29, 2022; published online April 20, 2022

There is high interest in the synergism of thin-film and flexible electronics with additive manufacturing. This review primarily focuses on the
prospective developments in convergence with flexible electronics manufacturing technologies. Specifically, this paper covers the latest 3D printing
and hybrid manufacturing technologies, the utility of specific types of materials, their functionalization and characterization, post-processing and
testing strategies toward fabricating robust and application-specific flexible electronics. Besides exploring the advances in this area of research—it
also highlights the limitations and gaps that have been observed in the previous years that will challenge and offer opportunities for advancing
research and development. Lastly, the future of 3D-printed flexible electronics is discussed in the aspects of customizability, scalability, and its
game-changing and state-of-the-art potential for intelligent sensing, instrumentation, and wearables for various medical, engineering, and
industrial applications. © 2022 The Author(s). Published on behalf of The Japan Society of Applied Physics by IOP Publishing Ltd

often synonymous with the term additive manufacturing (AM).

1. Introduction In several review papers, we recently reviewed advances in 3D
Flexible electronics are a class of electronic devices that printing methods, materials, including 3D printing for
commonly have substrates characterized and made of thin or electronics,10) mechanical testing,11) high-performance polymer
long stretchable materials.1) At a certain degree, it can be composites,12) graphene and polyurethane,13) stereolithographic
folded, stretched, elongated, rolled, or bent to either adapt to apparatus (SLA) 3D printing,14) thermoplastic composites,15)
specific rugged applications or to trigger changes in electrical graphene and SLA,16) carbon black and selective laser sintering
signals from changes in stimulus like how a sensor works.2) (SLS),17) silicone elastomers,18) hydrogels,19) and viscoelastic
The concept of such a class of conformable electronics has materials.20) In this case, AM could refer to a build-up of layered
existed ever since the first electronic devices were invented. or multi-layered structures that build on multi-materials or a
What sets it apart from any other electronics class is its computer-aided design (CAD) framework design origin. 3D
flexibility (more mechanical) when the application calls for it. printing in flexible electronics could be a combination of CAD-
From when flexible solar cells and thin-film transistors3) based layer addition and a more serial plug-and-place or pick-
started gaining ground around the late 1970s to their and-place design to construct a device.
significant contributions to biosensors in the last decade, The purpose of this review is to provide a fresh and
the way these are fabricated had to revolutionize the concise overview of the recent advances, grand challenges,
traditional manufacturing processes. Although the actual and prospects in the advanced manufacturing of flexible
electronic part itself may still conform to conventional electronics. This paper mainly covers the processing and
electronic device fabrication methods, the challenge has functionalization of materials, post-processing and testing,
always been its integration into its flexible substrate.1) 3D printing technologies and hybrid approaches, the newest
Flexible electronics, as it becomes a popular class of the family of flexible devices, and sustainability aspects of
electronics industry, likewise demands “flexible” ways of flexible electronics.
fabricating them that address the integrative approach to
customizability and application-specific needs.4) One innovative 2. Advances in manufacturing flexible electronics
way to push the limits in manufacturing of flexible electronics 2.1. Processing and functionalization of materials
has been the use of advanced methods of manufacturing such as Recent advances in flexible electronics enabled researchers
3D printing, wherein it opens a whole new manufacturing and electronics industry professionals to develop different
process and breed of products, such as wearables,5) processing techniques and functionalization of its materials.
biosensors,6–8) conformal antennas,9) and flexible energy har- Among the popular processing techniques to fabricate
vesters and storage,10) that somehow heed the demand for flexible electronics are transfer printing technology (TPT),
custom-built application-specific devices from the fields of two-dimensional printing (2D printing), and three-dimen-
medicine, renewable energy, and engineering. 3D Printing is sional printing (3D printing). Figure 1. illustrates the

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Jpn. J. Appl. Phys. 61, SE0803 (2022) PROGRESS REVIEW

(a) (b)

(c)

Fig. 1. (Color online) Figure 2.1(a) Schematic illustration of non-deterministic transfer printing of LED chips with controllable pitch using a pillar-patterned,
stretchable elastomeric stamp,24) (b) Schematic view of ink-based deposition schemes: droplet jetting and continuous filament writing,25) and (c) 3D Printing
Conductive Polymer Hydrogels.26)

difference in the setup for TPT, 2D printing, and 3D printing. The functionalization of flexible electronics can be done by
TPT is a widely used technique to manufacture flexible in situ polymerization,30) post-polymerization/coating,31) ad-
electronics through reversible interfacial adhesion of rigid dition of conductive particles,32) and ionic conductivity.33)
functional devices with elastomeric substrates.21,22) The 2D 2.2. 3D Printing
printing utilized 2D functional ink or liquid-based/aqueous Numerous studies and review articles demonstrate the
electrolyte integrated into the system as sensors, biosensors, applications of 3D-printed flexible electronics. These appli-
wearable displays, and other smart applications.23) For 3D cations include robots, pumps, wearables, energy absorption,
printing flexible electronics, the process involves 3D molded biocompatible materials, and different types of sensors
interconnected devices (3D-MID) that require printing of (piezoelectric, piezoresistive, bending sensors, electronic,
complex 3D structures and substrate geometries.10) strain sensors, capacitive force sensors, etc.), and many
The process of using 3D printing in flexible electronics is others.34) Several examples of these applications that are
dependent on the complexity of its design and the 3D manufactured using only a single 3D printing process are
printing technology that will be utilized. A preset pattern briefly discussed in this section,13,35–40) while those with two
that directly targets the substrate during printing is a complex or more processes (i.e. hybrid)41–44) are discussed in the next
process involving smart interactive operations between op- section. Table I summarizes the materials and technologies
erators and 3D printers.27) Hoerber et al. demonstrated in used in the 3D printing of flexible electronics. It should be
their research the enhanced process for building 3D devices mentioned that a key ingredient in flexible electronics is the
by aerosol jet printing and powder bed-based printer. Both flexibility of the substrate and therefore the use of materials
methods involve the integration of surface mount technology such as polyurethane (PU), silicone, or polydimethylsiloxane
(SMT) components into the structure. In aerosol jet printing, (PDMS), natural rubber, and other thermoset and thermo-
the SMT components were integrated into the structure via plastic elastomer compositions.
assembly and interconnection. While in a powder bed-based Christ et al.35) reported successfully having 3D-printed a
printer, the SMT components were buried into the powder flexible and conductive thermoplastic-based strain sensor.
bed with the cavities created during the process.28) They compounded thermoplastic polyurethane with multi-
Surface functionalization of flexible electronics is a walled carbon nanotube (TPU/MWCNT); filaments were
method to introduce electrical conductivity and optical extruded as fused deposition modeling (FDM) was used for
properties to attain its intended electronic application.29) the 3D printing of the sensor. The electrical, mechanical, and
© 2022 The Author(s). Published on behalf of
SE0803-2 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SE0803 (2022) PROGRESS REVIEW

Table I. Flexible electronic devices manufactured using different 3D printing technologies and materials.

Material 3D printing technology Application

35)
Thermoplastic polyurethane/multiwalled carbon nanotube (TPU/MWCNT) FDM Sensors
PDMS, TPU, silver micro flakes, NaCl crystals36) Extrusion Stretchable piezoresistive sensor
Rigid polyurethane and flexible Polyurethane37) Direct laser synthesis Bladder pumps, shape-to-fit
flexible wearables
polyurethane and a conductive filament38) FDM Multifunctional flexible bending
sensors
Conductive filament (Polycaprolactone with carbon black)39) FDM Electronic sensor
Thermoplastic polyurethane (TPU)40) FDM Energy absorption
Thermoplastic polyurethane (TPU)13) FDM Biocompatible materials/bioma-
terials scaffolds for tissue en-
gineering
Conductive polydimethylsiloxane (PDMS)41) Embedded 3D printing (e-3DP) Strain sensors
Photoresist and oil, with chromium and copper metallic layers42) 3D Microprinting/direct ink writing 3D conductive serpentine mi-
(DIW) crostructures/networks
Acrylonitrile butadiene styrene, conductive electrodes, and dielectric layer43) FDM, fiber encapsulation additive Acrylonitrile butadiene styrene,
manufacturing (FEAM), and ther- conductive electrodes, and
moplastic elastomer additive manu- dielectric layer
facturing
Tellurium and silver5) Aerosol jet printing and extrusion Piezoelectric sensor
printing
44)
Soft materials (multiple materials); PDMS EMB3D and molding Soft robot

piezoresistive properties were investigated under monoto- use of high-resolution printing and lattice structures can mini-
nous and cyclic loading conditions. MWCNTs increased the mize the structural support of flexible electronics.48)
stiffness of the TPU for better printability. The elastic Thermal post-processing is needed to evaporate the solvent
modulus slightly decreased, and there was no significant in ink. Usually, the process of annealing, laser curing, plasma
change in the material’s conductivity compared with the bulk treatment, and chemical sintering can be employed to
materials. A high piezoresistivity gauge factor has been eliminate electrically non-conductive organic additives and
measured even under 100% applied strains. Under cyclic surfactants that contribute to the increased resistivity in the
loading, a highly repeatable resistance strain response was electronics.23) Among the thermal post-processing, laser
observed. These characteristics demonstrate the potential sintering can conveniently be embedded in the printing
applications of such composite material in wearables, soft process to prevent the warping of 3D-printed flexible
robotics, and the like. Wei et al. similarly described the devices.10)
preparation of the reprocessable 3D-printed conductive To demonstrate the capability of flexible electronics with
composite foam of polyurethane (carbon black composite) external stimuli response, a triangular strain cycle can be
for strain and gas sensing.45) applied to the strain sensor via a universal testing machine.48)
Bates et al. successfully 3D-printed hyperelastic cellular The strain sensor is connected to a digital multimeter to
arrays, or what they called honeycombs, with graded monitor the changes in its resistance. The same approach can
densities for energy absorption.40) TPU was used to manu- be done by monitoring the voltage drop of the pressure
facture hexagonal arrays via FDM. Density grading was done sensor.49) Other than flexible electronics’ strain and pressure
by varying cell wall thickness through the specimen thick- sensing characteristics, other real-time applications such as
ness. Samples were subjected to static compression tests pulse monitoring, liquid evaporation monitoring, Morse
where the stress-strain behavior, efficiency-stress behavior, code, etc. are also becoming popular.47)
and energy absorption diagrams were obtained. The re- 2.4. Hybrid technologies and systems
searchers observed that by grading the density through the To achieve certain characteristics specific to electronic
specimen thickness, the structures were able to absorb higher applications, multiple or hybrid manufacturing may be
total energy under compression loading than the equivalent necessary to accommodate such needs. For example, Saari
uniform array. Further, they observed that the graded et al. used fiber encapsulation additive manufacturing
structures demonstrated higher efficiency at absorbing low (FEAM) and combined it with thermoplastic elastomer
energy compression loads than the equivalent uniform array. additive manufacturing (TEAM) to produce a composite
Lastly, they reported that the continuously graded array had capacitive force sensor.43) FEAM and TEAM are both AM
the highest efficiency over a wide range of compression processes that may be utilized to fabricate integrated elec-
energies. In contrast, the highest peak efficiency was ob- trical components and soft thermoplastic elastomers, respec-
served in the equivalent uniform density array. tively. The researchers produced a sensor with a 3D-printed
2.3. Post-processing and testing rigid frame, and wires with spiral patterns are embedded on
There are several techniques in post-processing 3D-printed the said frame. The sensor also has a dielectric spacer made
polymers46) but the most common method for complex 3D- of a thermoplastic elastomer that compresses upon applying
printed structures is the removal of support structures.47) The force. They investigated the capacitance change versus the
support structures are usually made from different materials and applied uniaxial compression load to evaluate the effective-
can be dissolved from the completed object post-printing.26) The ness of the capacitive force sensor.

© 2022 The Author(s). Published on behalf of

SE0803-3 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SE0803 (2022) PROGRESS REVIEW

Wehner et al.44) used molding and soft lithography to materials engineering, electronics architecture, robotics, auto-
fabricate the body and the microfluidic logic of a robot, mation, Artificial Intelligence, and process optimization.55)
respectively. In contrast, they used a multi-material em- One example presented by Kunnari et al.56) is the printing
bedded 3D printing method (EMB3D) to produce or pattern of a wristband. The researchers assessed the environmental
the other parts needed for movements, such as the catalytic impacts of inkjet printing (using a preliminary screening
reaction chambers and onboard fuel reservoirs. They con- approach) and compared it with the traditional process using
cluded that these combinations of materials and manufac- a printed wiring board. They also evaluated the inkjet-printed
turing technologies could be applied in soft, autonomous interconnections and compared them with the other parts of a
robots. Table I summarizes 3D printing technologies and prototype product. They observed that it is possible to make
materials to manufacture flexible electronic devices for electronics printing consume less energy than the traditional
specific applications. method. However, they claimed that more information is
2.5. 4D Printing needed (e.g. process-specific data for both the materials and
Shi et al.50) defined 4D printing as “the change of shape, printing processes), specifically, the manufacturing data for
property, and functionality from a 3D-printed structure the ink and nanoparticle. Factors such as printing speed,
response to time or external stimulus.”51) These stimuli substrate cleaning, and yield should all be considered for the
include water, heat, light, and pH.50) With the abovemen- printing itself. Optimization of all the involved processes is
tioned capabilities, 4D-printed parts have been popular for needed before claiming that the printing process is envir-
soft electronics, soft tactile sensors, actuators, etc. onmentally friendly. Another involves the possibility of using
Zarek et al. fabricated shape memory objects intended for biobased additives or feedstocks as in the use of nano-
responsive and flexible electrical circuits through 3D printing cellulose and cellulose-based composites57,58) or hydrogel
of methacrylated monomers. These responsive objects may inks59) for sustainable 3D printing materials.
be used for sensors, soft robotics, minimally invasive medical In the next section, the authors elaborate on the biggest
devices, and wearable electronics.52) Advincula and his team challenges we face in advancing the manufacturing of
have recently published the 4D printing of an epoxy/poly- flexible electronics and how the future might look as we
benzoxazine copolymer and CNT composite that exhibited address some of these challenges and take on research and
high thermal stability and shape memory printing.53) Wu et development advancements.
al.54) designed a 4D-printed flexible integrated magneto-
electric tactile sensor. The tactile sensor demonstrated a 3. Challenges and prospects
piezoelectric property (i.e. converting the external pressure Flexible and printed electronics carry opportunities and
into electric energy) even without any piezoelectric parts. The challenges for new materials and function development.
sensor consists of two parts. The first part is a porous The actual development of integrated devices has been
structure fabricated by SLS using TPU/NdFeB composite possible. Still, shape conformality, high performance, and
powders. The second part is a helix structure with two flat operating environmental considerations will always necessi-
plates fabricated by Selective Laser Melting (SLM) using 316 tate optimized research and development protocols for high
stainless steel powders. The device assembly can transfer technology readiness level requirements.1,55) There is also the
mechanical to electrical energy (and is based on the electro- need to have a hierarchy of fabrication and assembly methods
magnetic introduction principle). With the self-powered, that will require multi-materials approaches from metals,
sensitive, and quick-responding properties, this 4D-printed semiconductor films, conductive inks, and nanocomposite
tactile sensor may be used as a pressure sensor applicable to active and passive components.4,10) The use of elastomers for
warn against illegal invasion. This study also provides a new flexible shape conformality should be married with the
concept for the functionality-changed and property-changed environment and chemical resistance against degradation of
4D printing. performance.42,49,52) The materials’ processing conditions
2.6. Sustainability aspects and intrinsic development of structure-composition-property
An electronic circuit could be found in many devices we use will determine the structural hierarchy from nano- to micro-
daily. It would be essential to manufacture these devices and and macroscopic structures. Thermo-mechanical properties
electronic components considering aspects related to sustain- based on tensile, compression, and flexural modulus will be
ability (e.g. green energy, production efficiency, green integrated with the semiconductor and resistance properties
environment, life cycle assessment, industry 4.0, etc.). The of the conducting elements and will have defined actuation
traditional method of manufacturing electronic circuits in- movement.10) These are the possible requirements for unique
volves multiple production steps and consumes much energy wearable and soft-robotics types of applications.
aside from using toxic/corrosive etching chemicals to remove Here is an overview of the prospects on research trajec-
unwanted photoresist materials. On the other hand, novel tories for flexible electronics, as summarized in Fig. 2. The
manufacturing by digital printing reduces the manufacturing figure shows that there can be two major directions that will
steps, energy consumption and waste production. It does not continually inform each other: the tunability of characteristics
require etching, as only the needed material is selectively of flexible electronic devices and the innovative manufac-
deposited where it is required. Printing electronics is a turing methods.
disruptive innovation method that manufactures electronic 3.1. Flexural properties and sustainable materials
components used for many devices, including solar panels, New thermoplastic and thermoset elastomer composites that
energy harvesters, photovoltaic cells, and various sensors. take advantage of sustainable materials, e.g. biobased mate-
Printing of electronics requires a transdisciplinary research rials, natural fibers, that take advantage of the cost and
and production environment of different fields such as sustainability engineering with proper life-cycle analysis and
© 2022 The Author(s). Published on behalf of
SE0803-4 The Japan Society of Applied Physics by IOP Publishing Ltd
Jpn. J. Appl. Phys. 61, SE0803 (2022) PROGRESS REVIEW

performance conductivity, thermo-mechanical properties, and

actuation performance in specific operating environments.62)
4. Conclusion
This review aims at contributing to the body of knowledge on
flexible electronics by providing a brief overview of its recent
developments, methods and technologies for manufacturing,
materials processing, post-processing and testing, state-of-the-
art applications, the major challenges, and the future of research
in this area. Previous and current researchers have come to a
consensus that the biggest challenge lies in sustaining, tuning,
and improving its flexural characteristics. In addition, further
research and interdisciplinary inquiry are needed to explore
Fig. 2. (Color online) Potential research directions for flexible electronics.
novel characterization and fabrication techniques, optimized
design processes, and formulation and functionalization of
overall techno-economic analysis (TEA) of renewable or materials with tunable properties, and sustainability aspects that
recycled materials in conjunction with the AM methods. necessitate pushing for innovation and that would cater to the
3.2. Multifunction control and a new breed of evolving demands for specific applications from the industry,
composites and the fields of biomedicine, sciences, and engineering.
Multifunctional utility, i.e. combined optical and acoustic
Acknowledgments
sensing, electro-optical modulation, wireless multi-frequency
communication, etc. This should be paired with appropriate The authors would like to thank the Case Western Reserve
linear versus non-linear thermo-mechanical behavior as a University and the Department of Science and Technology—
flexible substrate with both synthetic and bio-based polymers Philippine Council for Industry, Energy and Emerging
sources. The use of fiber composites, e.g. C-fiber, Kevlar, PP Technology Research and Development (DOST-PCIEERD)
fibers, natural fibers, etc. as integral strengthening materials for the springboard support that fueled our research efforts on
in elastomers will be explored. the area of additive manufacturing. The authors also ac-
3.3. Bioinspired design and 4D printing knowledge funding support from the Governor’s Chair
3D printing with bioinspired design and function that draws Funds, University of Tennessee system, and ORNL’s
inspiration towards various applications and new structure- Center for Nanophase Materials Sciences under the US
composition-property relationships.32) For example, stimuli Department of Energy Office of Science User Facility.
response, e.g. motivation from metamorphic bone and
exoskeleton structures, color-or shape-changing in marine ORCID iDs
organisms, and controlled wetting behavior in insects, plants, Alejandro H. Espera Jr. https://orcid.org/0000-0002-3294-
and animals. All could lead to new wearable device designs 1847
and electronic functions, which may lean more towards the Rigoberto C. Advincula https://orcid.org/0000-0002-2899-
direction of 4D printing.60) 4778
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