BIOSENSORS
BIOSENSORS
BIOSENSORS
Review
Recent Progress in Manufacturing Techniques of
Printed and Flexible Sensors: A Review
Dinesh Maddipatla * , Binu B. Narakathu and Massood Atashbar
Electrical and Computer Engineering Department, Western Michigan University, Kalamazoo, MI 49006, USA;
[email protected] (B.B.N.); [email protected] (M.A.)
* Correspondence: [email protected]; Tel.: +1-269-276-3148
Received: 27 October 2020; Accepted: 29 November 2020; Published: 3 December 2020
Abstract: This review provides an outlook on some of the significant research work done on printed
and flexible sensors. Printed sensors fabricated on flexible platforms such as paper, plastic and textiles
have been implemented for wearable applications in the biomedical, defense, food, and environmental
industries. This review discusses the materials, characterization methods, and fabrication methods
implemented for the development of the printed and flexible sensors. The applications, challenges
faced and future opportunities for the printed and flexible sensors are also presented in this review.
Keywords: additive manufacturing; inkjet printing; screen printing; gravure printing; flexography
printing; flexible sensors; roll-to-roll manufacturing
1. Introduction
Sensors, which represent the “ears”, “noses”, or “eyes” for information processing systems,
are being widely used in numerous industrial applications as well as in our day-to-day lives. Sensors
are typically employed to provide real-time information, which has helped in advancing the electronic
industry by simplifying modern technical systems and making many technical applications more
cost effective, reliable, and safer. The need for sensing technologies has seen a dramatic increase
in sensor R&D and applications over the past 25 years [1–3]. The remarkable advances in sensing
technology, which have already been made possible and the potential range of applications that are
yet to be developed, have placed sensors on the threshold of a revolution similar to that experienced
by silicon technology in the computing industry during the 1980s [1,4]. An increasing demand
for miniaturized, cost effective, and reliable sensors capable of monitoring multiple environmental,
physical, chemical, and biological parameters thus requires the development of novel sensing devices
with advanced capabilities.
Flexible hybrid electronics (FHE) is a rapidly emerging field, with significant commercial potential
that drives investments in research and development within the electronic manufacturing industry [5,6].
FHE draws upon two primary threads: printed electronics (PE) and other advanced deposition/assembly
processes, and semiconductor devices and packaging technologies [7,8]. FHE devices are a natural
bridge between the silicon driven IC industry and the PE industry. Printing is an additive process that
has expanded into electronic applications where electronic materials are deposited selectively using
electrically functional inks in combination with standard printing processes [9–15]. This eliminates
the need for masking and etching, thus resulting in a cleaner process that produces less waste than
traditional methods. Due to the universal application of FHE technology, FHE markets are expected to
experience exponential growth over the next decade with a global market for consumer and industrial
products manufactured using this technology of up to $3 billion USD by 2030 [16].
The last few years have seen a noticeable increase in the development of wearable technology
devices that are often worn on the human body [17–20]. These devices provide the user with information
about various physiological parameters and surroundings. Currently, some of the markets for wearable
devices are in sports, fitness, and healthcare [21,22]. Examples of these applications include Nike’s
Fitbit exercise tracking and monitoring device and google contact lenses for diabetics that will provide
a continuous readout on blood glucose levels [23–26]. The wearable tech market is forecasted to reach
$302.3 million by 2023 [27]. More recently, with the advent of FHE devices, wearable devices that
integrate novel flexible, stretchable or even tattoo-like sensors, consisting of stretchable electrodes and
interconnects, which enable conformal and intimate skin-device contact, have been a major focus of
several research groups and companies [17,20,28–30]. The development of these devices includes the
deposition of functional materials on conformal and/or non-curvy surfaces in various designs.
The two main approaches in developing printed electronic devices are contact and non-contact
printing [31]. In the contact printing approach, ink is transferred from the surface of patterned
structures to the substrate by physical contact. Gravure, screen, and flexography printing are examples
of contact printing processes [31,32]. In a non-contact process, the ink is transferred to the substrate
via nozzles or openings, with no physical contact with the substrate. Inkjet and aerosol printing are
frequently used for non-contact printing [31,32]. The emergence of FHE based on PE has started
to increasingly revolutionize the field of sensing; both in industrial and consumer settings [33,34].
Flexible sensors can be used for curved surfaces, complex geometries, and foldable applications.
In contrast, rigid sensors fabricated by conventional microelectronics techniques cannot provide
the expected/desired responses on non-flat surfaces similar to the flexible sensors. In recent years,
the efforts to gain a better understanding of the dynamics of printing flexible sensors has increased,
and this interdisciplinary approach addresses the challenges of fabricating miniaturized, low-cost,
flexible sensors via high-throughput techniques, which are expected to be used for applications
in aerospace, automotive, environmental, packaging, biomedical, and defense [35–39]. PE enables
fabrication of cost-effective sensors via large area printing due to roll-to-roll manufacturing capability
utilizing solution-process techniques, large area substrates, multiple device printing per print batch,
and fabricating in ambient conditions [36–41]. Modern fabrication technologies and the rapid
maturation of application-based methodologies in PE have led to an increased understanding of
semiconductor analyte interactions for use in chemical and biological detection. In addition, various
types of physical sensors, such as strain sensors, optical sensors, temperature sensors, pressure sensors,
and chemical sensors, including electrochemical sensors and gas sensors, have been realized using
printing processes [42–48].
This review provides a detailed study on the dynamics of the PE by involving some common
printing techniques, key materials and substrates, fabricated sensor types, challenges, and opportunities
in the printed flexible sensors area. This review has the following structure: Section 2 discusses
printable electronic materials and appropriate substrates, some important characterization methods
to be considered for pre-print compatibility of materials and post-print quality analysis/assessments.
The description of some commonly used non-contact and contact printing processes utilized for
depositing solution-based materials and some examples of physical and chemical printed sensors
will be discussed in Section 3. Finally, Section 4 brings together the technical challenges faced in the
utilization of printing processes for the fabrication of flexible sensors and the opportunities enabled by
the printing processes will be discussed.
2.1. Substrates
Printed electronics often require substrates that are uniform in smoothness, solvent resistance,
stretchable, conformal, flexible, and light weight while providing both chemical and thermal stability.
The substrates that are commonly used for fabricating FHE devices are poly (ethylene terephthalate)
Biosensors 2020, 10, 199 3 of 24
(PET), polyimide (PI), thermoplastic, polyethylene naphthalate (PEN), and thermoplastic polyurethane
(TPU) [49–52]. As shown in Table 1, these substrates have different properties in terms of thickness,
glass transition temperatures (Tg ), and transparency (for optical-based applications). In addition to
these substrates, paper (specifically for fabricating disposable devices) and polydimethylsiloxane
(PDMS) have also been employed for fabricating PE-based sensors and devices [49,52,53]. Each of
these substrates is chosen for a particular application based on its properties. For example, PET excels
in applications that require a very smooth surface of a few nanometers and optical transparency.
PI substrates are widely employed for fabricating flexible PCBs due to their high glass transition
temperatures and relatively higher mechanical as well as chemical strength, when compared to PET [54].
TPU and PDMS substrates are popular for developing stretchable devices, whereas as paper substrates
are more common for developing cheap and disposable devices [55–57]. However, paper and TPU
have a relatively higher surface roughness (≥ 1 µm) compared to other substrates [58].
2.2. Inks
The basic components of an ink system consist of functional elements, binders, solvents,
and additives (Table 2) [59]. Typically, materials such as metals, semiconductors, and dielectrics
are used as functional elements [59,60]. The most used metallic material, as a functional element,
is silver (Ag) in the form of flakes, nanowires, and nanoparticles with a conductivity of ≈105 S/m,
which can be even improved using optimized annealing processes [61]. Carbon nanotubes (CNTs),
carbon black (C), and graphene have also been used as functioning elements for different applications,
including electrochemical sensing, humidity sensing, temperature sensing, and energy storage with
a maximum conductivity of ≈102 –103 S/m [62,63]. In recent years, research has been focused on
using copper (Cu) (which is abundantly available and relatively cheap) as a functional element for
metallic inks to replace Ag [64]. In addition to this, nickel (Ni), metallic composites (Ag/C), indium
tin oxide (ITO), have also been used as conductive functional elements [65–67]. Semiconductors
such as poly(3-hexylthiophene) (P3 HT); titanium dioxide (TiO2 ); zinc oxide (ZnO); and dielectrics
such as poly (methyl methacrylate) (PMMA), barium titanate (BaTiO3 ), polyvinyl pyrrolidone (PVP),
polydimethylsiloxane (PDMS), and poly urethane (PU) have also been used as functional elements
based on the application needs [59,65,68].
The other components of the ink system such as binders, solvents and additives, facilitate
functional elements’ printability on flexible platforms [59,68]. Typically, binders are mixed with the
functional elements in the presence of a compatible solvent, and they provide uniform film formation
by crosslinking the functional elements after a curing process (thermal, UV or sintering) [59,68].
In addition to film formation, binders also provide the adhesion required for functional elements with
the substrate along with gloss and resistance to humidity or ambient light conditions [59,68]. Cellulose-,
alkyds-, rubber-, and acrylic-based resins have been used widely as binders. Water and a wide range
of organic solvents including aromatic hydrocarbons, ethyl acetate, and alcohols (ethanol, isopropyl
alcohol, etc.) have been used as solvents in the ink systems [59,68]. The solvents either uniformly
dissolve or disperse the other components of the ink systems, facilitating the easy application of ink
fluids on to the printing systems [68]. Recently, water-based inks have been gaining more attention due
to low evaporation rates, low costs, and non-toxic nature [68,69]. Additives are used to modify/tweak
certain ink systems’ properties in terms of wettability, surface tension, and pH [59,68]. For example,
water-based inks have high surface tension, and surfactants as well as defoamers are used to reduce the
surface tension and improve the wetting characteristics of the ink system [70]. In addition, humectants
(hygroscopic material) are also used as additives to reduce the evaporation rates of the solvent in the
ink system [68]. Multiple parameters must be considered when designing the ink system components
in order to achieve a uniform ink film with desired characteristics without any coffee-ring effects and
ink spreading that results in high raggedness.
Biosensors 2020, 10, 199 4 of 24
2.3.1. Rheometry
Rheology is the study of flow and deformation of fluid materials under applied forces (created
due to stresses applied on it) [59,68]. It provides information on the behavior of the fluid systems under
stresses, which is important in determining the compatible printing process, storage conditions (shelf life,
anti-settling, and re-dispersibility), formulation (dispersion quality, stability, and viscosity adjustment)
and quality of final film (thickness, smoothness, flow as well as levelling, and uniformity) [59,74–76].
Fluids can be typically classified as Newtonian and non-Newtonian fluids [77,78]. In Newtonian
fluids, viscosity is constant over a wide range of shear rates and stress [77,78]. They have a single
coefficient of viscosity for a specific temperature. On the contrary, non-Newtonian fluids cannot be
defined by a single viscosity value, and they exhibit a variety of different correlations among viscosity,
shear rate, and shear stress [77,78]. Typically, the ink fluid systems used for printed electronics are
non-Newtonian fluids [79]. A device known as a rheometer is used for characterizing the rheological
behavior of non-Newtonian fluids that require more parameters including shear stress, shear rate,
and temperature to be set/varied to measure the corresponding variations in the viscosity values over
time [76,80]. Typically, high viscosity inks ranging from 0.5 Pa.s. to 60 Pa.s. that exhibit thixotropic
behavior are required for screen printing. Thixotropy is defined as the ability of the ink to exhibit
relatively low/reduced viscosity, temporarily upon the application of shear, and then recover to its
original/initial state (higher viscosity) when the shear is removed; thixotropic behavior facilitates the
ink flow through the screen mesh resulting in ink transfer to the substrate and thus leads to ease of
processability [66]. The gravure and flexo requires ink systems with viscosities ranging from 0.01 Pa.s.
to 1.1 Pa.s. and 0.01 Pa.s. to 0.5 Pa.s., respectively, also typically thixotropic. In inkjet printing,
for proper drop formation and jetting, viscosity of the ink should be below 0.1 Pa.s., which also may be
thixotropic [31,66,81].
(a) (b)
Figure
Figure 1. (a)1.Illustration
(a) Illustration of intermolecularattractive
of intermolecular attractiveforces
forces in
in aa droplet
droplet and
and (b)
(b)wetting
wettingbehavior
behaviorof of
liquid
liquid drop-based
drop-based on contact
on contact angle.
angle.
Optical profiler and laser interferometry, scanning electron microscope, atomic force microscopy,
Fourier transform infrared spectroscopy, X-ray fluorescence, and X-ray diffraction techniques are
typically used to study the surface characteristics. In post-printing processes, many of these techniques
are used to measure and analyze the structural properties, thickness, and roughness of the printed ink
as well as print quality details such as raggedness and resolution.
There are many flexible circuits, electronic devices, and sensors fabricated using screen
printing process, and their functionality has been demonstrated with performance comparable
to traditional/conventional devices. For example, Eshkeiti et al. fabricated prototypes of multilayered
printed circuit boards (PCBs) prototypes with Ag and UV acrylic inks as metallization and dielectric
layers, respectively using AMI 485 semi-automatic screen-printing press [93]. They were the first
research group that implemented fully operational three-layered flexible PCB prototypes on PET
(Figure 2b), glass (Figure 2c) and paper (Figure 2d) substrates with electronic components and
microcontroller populated using pick and place equipment to drive a liquid-crystal display of
160 × 100 pixels. The resistance of the printed lines increased by only ≈1.8%, after subjecting to
10,000 cycles of bending indicating the robustness of the printed and flexible PCB prototype. Cao et al.
reported the first fully fabricated screen printed top-gated TFTs using semiconductor-enriched SWCNT
as channel materials, Ag as source, drain as well as gate, and high-k barium titanate as dielectric layer on
PET substrate [94]. The TFTs had a mobility up to 7.67 cm2 V−1 s−1 with low operating voltage of less than
10 V and current on/off ratio between 104 –105 with superior mechanical flexibility. They demonstrated
the capability of the printed TFTs by controlling the intensity of external OLEDs shown in the inset
of Figure 2e. Three electrode configurations on PET and polyimide were screen printed with Ag, C,
and Ag/AgCl as counter, working and reference electrodes, respectively, by Dr. Atashbar’s research
group, to selectively detect various heavy metals including mercury, lead, cadmium, and copper in
drinking water (Figure 2f,g) [95–98]. These flexible and planar electrochemical sensors are compatible
with all types of traditional electrochemical techniques including cyclic voltammetry, amperometry,
and differential pulse voltammetry, and has detection capability well below the toxicity levels set by
the U.S. environmental protection agency (EPA) and world health organization (WHO). In addition,
the printed electrochemical sensor presented by Maddipatla et al. provided lower limit of detection
(LOD) and limit of quantification (LOQ) compared to colorimetric and optochemical sensors [98,99].
Emamian et al. successfully fabricated a complex piezoelectric-based touch sensor using screen
printing process [100]. The sensor consists of a polyvinylidene fluoride (PVDF)-based piezoelectric
layer sandwiched between the top and bottom Ag electrode layers. All these layers were completely
screen printed on PET (Figure 2h) and paper (Figure 2i) substrates, and the polarization of the PVDF
layer was investigated by performing capacitance-voltage analysis. The PET-based touch sensor
has a sensitivity of 1.2 V/N whereas paper-based sensor exhibited 0.3 V/N demonstrating that these
sensors have the potential to be employed as touch sensors or energy harvesters in robotics and
automotive applications. Various temperature, strain, and pressure sensors have also been realized
using additive screen-printing process. Turkani et al. reported nickel (Ni)-based resistance temperature
detector (RTD) on polyimide substrate for detecting wide range of temperatures varying from −60 ◦ C
to 180 ◦ C (Figure 2j) [101]. The flexible RTD exhibited a relative resistance change of 113% with a
temperature coefficient resistance (TCR) of 0.44%/◦ C and response time of <10 s. The thin RTD film
was also very stable and repeatable across the wide temperature ranges. Yoon et al. and Bose et al.
fabricated flexible and stretchable strain sensors using screen printing process by depositing Ag ink
on TPU substrates (Figure 2k) [102,103]. Multiple configurations including wavy, meander lines, and
horseshoe-type were used to detect the applied strains [102–105]. A 20% strain was detected by the
strain sensor with wavy configuration and demonstrated excellent stretchability when compared to
conventional strain sensors. These multiple research works demonstrate the feasibility of employing
screen-printing process for the development of various cost-efficient and high-performance electronic
devices, sensors, and circuits [106–109]. Currently, screen printing is one of the most employed
processes in the production lines of printed electronics.
Electrical and Computer Engineering Department, Western Michigan University, Kalamazoo, MI, 49006,
USA;
[email protected] (B.B.N.); [email protected] (M.A.)
* Correspondence: [email protected]; Tel.: +1-269-276-3148
Received:
Biosensors 2020,27
10,October
199 2020; Accepted: 29 November 2020; Published: date 9 of 24
Figure2.2.(a)
Figure (a)Schematic
Schematic ofof
screen
screenprinting
printingprocess;
process; screen printed
screen multilayered
printed multilayered flexible circuits
flexible on (b)
circuits onpoly
(b)
(ethylene terephthalate) (PET), (c) glass, (d) paper platforms [93], © IEEE, Reprinted
poly (ethylene terephthalate) (PET), (c) glass, (d) paper platforms [93], © IEEE, Reprinted with with permission
from IEEE Transactions
permission from IEEE on Components,
Transactions Packaging andPackaging
on Components, Manufacturing Technology; (e)
and Manufacturing screen printed
Technology; (e)
screen printed
top-gated top-gated TFTs,
TFTs, Reprinted Reprinted with
with permission [94], © American
from permission from [94], © American
Chemical Society;Chemical Society;
(f,g) flexible and
2 ) [98,99], Reprinted with permission
(f) and
planar (g) flexible and
electrochemical planaronelectrochemical
sensors PET and PI substratessensors (2on×PET
1 cmand PI substrates (2 × 1 cm2) [98,99],
Reprinted with permission from RSC and IEEE Sensors Journal; (h), and
from RSC and IEEE Sensors Journal; (h), and (i) polyvinylidene fluoride (i) polyvinylidene
(PVDF)-based fluoride
touch sensor on
(PVDF)-based touch sensor on PET and paper platforms, Reprinted from [100] with permission from
PET and paper platforms, Reprinted from [100] with permission from Elsevier; (j) Ni-based resistance
2 ) [101], © IEEE, Reprinted with
Elsevier; (j) detector
temperature Ni-based(RTD)
resistance temperature
on polyimide detector(2.5
substrate (RTD)
× 1.2oncm polyimide substrate (2.5 × 1.2 cm2)
[101], © IEEE,
permission from Reprinted with permission
IEEE Access; (k) flexiblefrom
and IEEE Access;strain
stretchable (k) flexible
sensors, andReprinted
stretchablefrom
strain sensors,
[102] with
Reprinted from
permission from Elsevier.
[102] with permission from Elsevier.
nozzle is mechanically deformed based on the image signal and the ink droplets are released from the
nozzle. DOD-based inkjet printing is very popular in FHE and has several advantages including as
mask-less fabrication, high print resolution, cost efficiency, and scalability from table-top devices to big
press units [90,110–112].
Various devices have been fabricated using inkjet printing process. Ochoa et al. developed
flexible paper-based continuous oxygen delivery and sensing bandage platform using inkjet printing
to treat chronic wounds (Figure 3b) [70,113]. The authors employed parchment paper as the base
platform of the dressing and inkjet-printed manganese oxide (MnO2 ) and ruthenium-based inks
on parchment paper for locally generating and measuring oxygen in a wound region. By varying
the density of the inkjet-printed MnO2 deposited, the generation of the oxygen concentration was
controlled. The fluorescence property of inkjet-printed ruthenium on the paper substrate facilitates
contact less measurement of oxygen at a wound site (Figure 3c) [114]. This multi-functional smart
wound healing bandage is designed as a wound dressing platform that offers various properties of
wound dressings (e.g., mechanical strength and flexibility) while featuring additional ones not found
in conventional wound dressings (e.g., on-site generation of oxygen, delivery of oxygen or other
therapeutics, and integration of sensors on the same substrate). Typically, wounds vary from one to the
other, and even the extent of tissue damage across any single wound site is not uniform and requires
different concentrations of oxygen and other therapeutics across the wound site. Implementation of
inkjet printing is very pivotal for this research due to its rapid, mask-less customization of designs for
accelerated dressing development as well as for mass customization. In other words, inkjet printing
facilitates rapid fabrication of customized wound bandages in terms of dimensions/size as well as the
intensity of the oxygen and other therapeutics to match the specific requirements (provided by the
clinicians) of an individual wound. The significance of this research is based on the contribution that
this project is bound to have towards the field of wound treatments [115].
Mikolajek et al. prepared fully inkjet-printed metal–insulator–metal capacitors (Figure 3d) [116].
They deposited Ag as metal electrodes and BST/PMMA as insulator or dielectric material on
PET substrate using inkjet printing process. This printing process deposited thin, very uniform,
and smooth layers with high resolution and relatively less pinholes. Therefore, the printed BST/PMMA
composite-based dielectric layer exhibited 7 to 18 times higher dielectric constant when compared to pure
PMMA. In addition, Li et al. fabricated graphene-based micro-supercapacitors using electrochemically
exfoliated graphene as electrodes and current collectors, and polyelectrolyte ink (made using
poly(4-styrenesulfonic acid) as a solid-state electrolyte (Figure 3e) [117]. The micro-supercapacitors
have an aerial capacitance of 0.7 mF/cm2 , and when connected in an array of over 100 devices on a
flexible polyimide substrate, the devices can be charged to 12 V. The super capacitors were able to retain
their performance over 8 months even without any encapsulation due to the use of polyelectrolyte ink.
Further, Cao et al. developed a multi-layered flexible organic Schottky diode on flexible PET substrate
using inkjet printing process (Figure 3f) [118]. Ag ink and poly(3,4-ethylenedioxythiophene) polystyrene
sulfonate (PEDOT:PSS) was used as bottom and top electrodes, respectively. A poly(3-hexylthiophene
(P3HT) was employed as a semiconducting layer sandwiched between the top and bottom electrodes.
A precise control on fine ink deposition and better ink flow which are very crucial for multilayer
devices was achieved by using inkjet printing and including microfluidic networks with capillary
channels and flow stoppers in the diode fabrication. The printed diodes exhibited a high rectification
ratio of 5 × 104 with negligible hysteresis and high durability in bending tests.
Bissannagari et al. developed a flexible wireless power transfer module using inkjet printing
process (Figure 3g) [119]. In this work, a 3D nickel (Ni)-Zinc (Zn)-ferrite (NZF)-based trench structure
hybridized with alternative layers of Ag and PI in a spiral pattern was created using inkjet printing
to fabricate a flexible power receiving coil. In addition, a resonance capacitor with Ag as top and
bottom electrodes; BaTiO3 and PI infiltrated BaTiO3 as dielectric layers was also fabricated using inkjet
printing process and integrated to power receiving coil in order to fine tune the resonance frequency of
the coil to 6.78 MHz. The coil with capacitor was embedded in to PDMS films using casting method
Biosensors 2020, 10, 199 11 of 24
to serve as encapsulant as well as to reduce the bending/physical stress on the coil. This wireless
module was able to successfully charge a mobile phone or a smart watch even at a distance of 40 mm.
Narakathu et al. developed flexible microfluidic-based sensing platforms in which the Ag-based
electrodes were inkjet-printed to detect and quantify various concentrations (as low as picomolar
levels) of toxic chemicals such as mercury sulfide and cadmium sulfide using impedance spectroscopy
(Figure 3h) [120]. Due to the attractive features such as mask-less fabrication and high print resolution,
various other devices such as SERS substrates for the detection of heavy metals, gas sensors, humidity
sensors, thermistors, and antennas were also realized using inkjet printing process [121–126].
Biosensors 2020, 10, x FOR PEER REVIEW 2 of 4
(i) (ii)
(iii)
(a)
(b)
(d) (c)
Figure 3. (a) Schematic of inkjet printing process; (b) flexible paper-based bandage with continuous
Figure 3. (a) Schematic of inkjet printing process; (b) flexible paper-based bandage with continuous
oxygen delivery and sensing capabilities developed to treat the chronic wounds: (i) overview illustration
oxygen delivery and sensing capabilities developed to treat the chronic wounds: (i) overview
of the patch in use for foot ulcer applications, (ii) cross-sectional view of oxygen generation and sensing
illustration of the patch in use for foot ulcer applications, (ii) cross-sectional view of oxygen generation
patch and wound area, (iii) mechanisms for generating and sensing oxygen on a flexible smart wound
and sensing patch and wound area, (iii) mechanisms for generating and sensing oxygen on a flexible
dressing [70]; (c) paper-based oxygen sensors [114], Reprinted with permission from RSC; (d) fully
smart wound dressing [70]; (c) paper-based oxygen sensors [114], Reprinted with permission from
inkjet-printed
RSC; (d) fullymetal–insulator–metal capacitors [116];capacitors
inkjet-printed metal–insulator–metal (e) graphene-based micro-supercapacitors
[116]; (e) graphene-based micro-
using electrochemically
supercapacitors exfoliated graphene
using electrochemically as electrodes
exfoliated graphene and
as current collectors,
electrodes Reprinted
and current with
collectors,
permission from [117], © American Chemical Society; (f) multilayered flexible organic
Reprinted with permission from [117], © American Chemical Society; (f) multilayered flexible organic Schottky
diode on PET
Schottky substrate
diode on PET [118], © IOP
substrate Publishing,
[118], Reproduced
© IOP Publishing, with permission
Reproduced from IOP;
with permission from (g)IOP;
flexible
(g)
wireless power transfer module (42 × 42 mm 2 ), Reprinted from [119] with permission from Elsevier;
flexible wireless power transfer module (42 × 42 mm2), Reprinted from [119] with permission from
(h) microfluidic-based
Elsevier; sensing platforms
(h) microfluidic-based with inkjet-printed
sensing platforms Ag electrodes
with inkjet-printed (3.8” ×(3.8″
Ag electrodes 2.5” ××2.5″
0.2”) [120],
× 0.2″)
©[120],
IEEE,©Reprinted with permission
IEEE, Reprinted from IEEE
with permission fromSensors Journal.
IEEE Sensors Journal.
Biosensors 2020, 10, 199 12 of 24
(a)
12 mm
(c) (b)
of functional inks compatible to flexographic printing. Therefore, there is only limited literature
available
Biosensors on the
2020, 10, development of flexography-based FHE devices [140–142].
x FOR PEER REVIEW 4 of 4
(a) (b)
(c) (d)
Figure5.5.(a)
Figure (a)Schematic
Schematic ofof flexography
flexography printing
printing process;
process;(b) (b)flexible
flexiblechip
chipless
lessRFID
RFIDtags tags(5-bit
(5-bitring
ring
2 2), 3-bit UH-strip tag (30 × 30 mm22 ) and 4-bit U-slot tag (34 × 16 mm 2 )) [138],
resonator tag (34 × 34 mm ), 3-bit UH-strip tag
resonator tag (34 × 34 mm × 30 mm ) and 4-bit U-slot tag (34 × 16 mm )) [138],
2
©© IOPPublishing,
IOP Publishing,Reproduced
Reproduced with with permission
permission fromfrom IOP;
IOP; (c)and
(c)and(d)(d)chiral
chiralnematic
nematicoxetane
oxetane liquid
liquid
crystals
crystals (LC)
(LC) on on
PETPET platform
platform (3 × (3
3 cm× 3), cm
2 2 ), Reprinted
Reprinted with permission
with permission from©[143],
from [143], © American
American Chemical
Chemical
Society; Society;
(e) high (e) high
mobility mobility
flexible flexible CNT-based
CNT-based TFTs on PEN TFTs on PEN(15
substrate substrate
× 15 cm(15 × 15 cm2) (2013)
2 ) [144], ©
[144], The
© (2013)
Japan TheofJapan
Society Society
Applied of Applied
Physics; Physics;
(f) fully printed(f)flexible
fully printed flexible
large area loudlarge area on
speaker loud speaker
a paper on a
platform
paper
(16 cm2 ),platform
Reprinted cm2),[145]
(16from Reprinted from [145] with
with permission frompermission
Elsevier; (g)from Elsevier;
Ag-based (g) Ag-based
strain sensors on strain
paper
sensors [146],
platform on paper platform
© IEEE, [146], ©
Reprinted IEEE,
with Reprintedfrom
permission withIEEE
permission
Sensorsfrom IEEE Sensors
Conference Conference
Proceedings.
Proceedings.
Shrestha et al. developed flexible chipless RFID tags using a benchtop flexography printer
(Figure 5b) [138]. Three resonators (3-bit UH-strip tag (30 × 30 mm2 ), 4-bit U-slot tag (34 × 16 mm2 ),
and 5-bit ring resonator tag (34 × 34 mm2 )) were fabricated by depositing water-based Ag ink on three
different substrates (PET, thermal paper, and PVC). The printed tags were evaluated for their microwave
performance, and the electromagnetic responses were used to obtain the tag IDs. The radar cross-section
amplitudes of the tags printed on PET demonstrated relatively better performance when compared to
the tags printed on other substrates. The three printed tags generated pre-defined resonances between
1–10 GHz in the unlicensed ultra-wide band frequency spectrum. Hoekstra et al. developed novel
photonic materials based on chiral nematic oxetane liquid crystals (LC) using flexographic printing
process for potential application as anticounterfeit labels (Figure 5c) [143]. To create the LCs, different
concentrations of oxetane-based materials were mixed with cationic photo initiators and deposited on
the biaxially oriented 36 µm PET substrate using flexographic printer. Then, the printed patterns were
Biosensors 2020, 10, 199 15 of 24
thermally cured to align the LCs and photopolymerized using a UV dryer. As shown in Figure 5d,
the patterns consist of both chiral nematic and isotropic regions with high resolution.
Higuchi et al. developed high mobility flexible CNT-based TFTs (Figure 5e) [144]. In this work,
they deposited Ag nanoparticle ink, polyimide ink and resist ink with Nmethyl-2-pyrrolidone (NMP)
solvent as electrodes (source, drain, and gate), gate insulator and CNT patterner, respectively on to a
plasma treated PEN film using flexographic printing process. The CNTs grown by chemical vapor
deposition technique was transferred on to TFT electrodes. The printed TFT exhibited a high mobility
of 157 cm2 /Vs with an ON/OFF ratio of 104 . Hubler et al. reported the first fully printed flexible large
area loudspeaker on a paper platform. PEDOT:PSS and poly(vinylidene fluoride-trifluorethylene
(P(VDF-TrFE)) was deposited as electrodes (top and bottom) and piezoelectric layer, respectively, on a
matt coated wood-containing paper using flexographic printing (Figure 5f) [145]. The P(VDF-TrFE) layer
was sandwiched between the electrodes, like a capacitor. The samples were polarized by contact-poling
process across an effective area of 16 cm2 . The speakers were able to generate 80 dB sound and exhibited
stable performance over six months in air without any encapsulation. In addition, Maddipatla et al.
developed a paper-based strain sensor using flexography printing (Figure 5g) [146]. The authors
printed Ag-based strain gauges with different meander lengths using pilot scale flexography press at
30 FPM. The printed flexible strain sensors, subjected to 3-point bend tests, were able to detect minute
displacements as low as 1 mm with repeatable performance over 500 cycles.
degrades the electronic performance of FHE devices. To overcome these major challenges that FHE
currently faces, the standardization of various parameters that could provide devices with high
reliability, repeatability, and robustness is required. In order to establish standards and mature the FHE
research area, a data cube must be developed with all the parameters that can impact the electronic
performance of each FHE device including simulation tools (to design, model, and simulate the
complete device), pre-print characterizations (viscosity, shear rate, surface tension, wetting properties
of ink, surface roughness, thickness, gas permeability, and defects in identification of substrate),
printing process parameters (deposition conditions of the printer, ambient temperature, and humidity),
post-print characterizations (print film thickness, roughness, coverage, raggedness, and functionality),
mechanical tests (bending, twisting, and flexing), and shelf-life characterizations (lifetime of each
material and the device). Around the globe, many manufacturing innovation institutes (NextFlex,
San Jose, CA, USA; HI-RESPONSE, Swindon, UK, and MADRAS consortiums, Barcelona, Spain,
Europe) are working in collaboration with numerous scientists and experts in both academia and
industry to address the challenges associated with the printing processes and set the standards to
advance the manufacturing ecosystems of the rapidly expanding field of FHE [153–156]. Adopting
these novel additive printing technologies on flexible platforms would potentially lead to cost-efficient
and flexible devices [157–160] and is being envisioned to revolutionize diverse applications in many
fields including food, agriculture, defense, automotive, and biomedical in the next few years.
Funding: This work was supported in part by the Flexible Hybrid Electronics Manufacturing Innovation Institute,
NextFlex, under U.S. Air Force Research Laboratory (AFRL) cooperative agreement #FA8650-15-2-5401, and in
part by the NSF PFI:AIR under award #1701157.
Conflicts of Interest: The authors declare no conflict of interest.
References
1. Anderson, G.; Anderson, G. The economic impact of technology infrastructure for smart manufacturing,
US Department of Commerce. Natl. Inst. Stand. Technol. 2016. [CrossRef]
2. Ho, C.K.K.; Robinson, A.A.; Miller, D.R.; Davis, M.J. Overview of sensors and needs for environmental
monitoring. Sensors 2005, 5, 4–37. [CrossRef]
3. Lymberis, A. Smart wearables for remote health monitoring, from prevention to rehabilitation: Current R&D,
future challenges. In Proceedings of the International IEEE EMBS Special Topic Conference on Information
Technology Applications in Biomedicine, Birmingham, UK, 24–26 April 2003; pp. 272–275. [CrossRef]
4. Wilson, J.S. Sensor Technology Handbook; Elsevier: Amsterdam, The Netherlands, 2004.
5. NEXTFLEX Gains $154M in AFRL Funding for 3D Printing Flexible Hybrid Electronics. Available
online: https://3dprintingindustry.com/news/nextflex-gains-154m-in-afrl-funding-for-3d-printing-flexible-
hybrid-electronics-172700/ (accessed on 12 September 2020).
6. Obama Administration Announces New Flexible Hybrid Electronics Manufacturing Innovation Hub in
San Jose, CA, USA. Available online: https://obamawhitehouse.archives.gov/the-press-office/2015/08/28/fact-
sheet-obama-administration-announces-new-flexible-hybrid (accessed on 12 September 2020).
7. FHE Technology & Markets. Available online: https://www.nextflex.us/about/about-fhe/ (accessed on
5 September 2020).
8. Khan, Y.; Thielens, A.; Muin, S.; Ting, J.; Baumbauer, C.; Arias, A.C. A New Frontier of Printed Electronics:
Flexible Hybrid Electronics. Adv. Mater. 2020, 32, e1905279. [CrossRef] [PubMed]
9. Maddipatla, D.; Zhang, X.; Bose, A.K.; Masihi, S.; Narakathu, B.B.; Bazuin, B.J.; Williams, J.D.; Mitchell, M.F.;
Atashbar, M.Z. A Polyimide Based Force Sensor Fabricated Using Additive Screen-Printing Process for
Flexible Electronics. IEEE Access 2020, 8, 207813–207821. [CrossRef]
10. Perelaer, J.; Smith, P.J.; Mager, D.; Soltman, D.; Volkman, S.K.; Subramanian, V.; Korvink, J.G.; Schubert, U.S.
Printed electronics: The challenges involved in printing devices, interconnects, and contacts based on
inorganic materials. J. Mater. Chem. 2010, 20, 8446–8453. [CrossRef]
11. Zhang, X.; Maddipatla, D.; Bose, A.; Hajian, S.; Narakathu, B.B.; Williams, J.D.; Mitchel, M.F.; Atashbar, M.Z.
Printed Carbon Nanotubes Based Flexible Resistive Humidity Sensor. IEEE Sens. J. 2020, 20, 12592–12601.
[CrossRef]
Biosensors 2020, 10, 199 17 of 24
12. Maddipatla, D.; Narakathu, B.; Turkani, V.; Bazuin, B.; Atashbar, M. A gravure printed flexible electrochemical
sensor for the detection of heavy metal compounds. Multidiscip. Digit. Publ. Inst. Proc. 2018, 2, 950.
[CrossRef]
13. Garlapati, S.K.; Divya, M.; Breitung, B.; Kruk, R.; Hahn, H.; Dasgupta, S. Printed electronics based on
inorganic semiconductors: From processes and materials to devices. Adv. Mater. 2018, 30, 1707600. [CrossRef]
14. Choi, H.W.; Zhou, T.; Singh, M.; Jabbour, G.E. Recent developments and directions in printed nanomaterials.
Nanoscale 2015, 7, 3338–3355. [CrossRef]
15. Chlaihawi, A.A.; Emamian, S.; Narakathu, B.B.; Ali, M.M.; Maddipatla, D.; Bazuin, B.J.; Atashbar, M.Z.
A screen printed and flexible piezoelectric-based AC magnetic field sensor. Sens. Actuators A Phys. 2017, 268,
1–8. [CrossRef]
16. Dyson, M.; Ghaffarzadeh, K. Flexible Hybrid Electronics 2020–2030: Applications, Challenges, Innovations
and Forecasts. IDTechEX. 2020. Available online: https://www.idtechex.com/en/research-report/flexible-hybrid-
electronics-2020-2030-applications-challenges-innovations-and-forecasts/732 (accessed on 9 October 2020).
17. Kim, D.H.; Ahn, J.H.; Choi, W.M.; Kim, H.S.; Kim, T.H.; Song, J.; Huang, Y.Y.; Liu, Z.; Lu, C.; Rogers, J.A.
Stretchable and foldable silicon integrated circuits. Science 2008, 320, 507–511. [CrossRef] [PubMed]
18. Jang, K.I.; Han, S.Y.; Xu, S.; Mathewson, K.E.; Zhang, Y.; Jeong, J.W.; Kim, G.T.; Webb, R.C.; Lee, J.W.;
Dawidczyk, T.J.; et al. Rugged and breathable forms of stretchable electronics with adherent composite
substrates for transcutaneous monitoring. Nat. Commun. 2014, 5, 1–10. [CrossRef] [PubMed]
19. Gao, W.; Emaminejad, S.; Nyein, H.Y.Y.; Challa, S.; Chen, K.; Peck, A.; Fahad, H.M.; Ota, H.; Shiraki, H.;
Kiriya, D.; et al. Fully integrated wearable sensor arrays for multiplexed in situ perspiration analysis. Nature
2016, 529, 509–514. [CrossRef] [PubMed]
20. Eshkeiti, A. Novel Stretchable Printed Wearable Sensor for Monitoring Body Movement, Temperature and
Electrocardiogram, Along with the Readout Circuit. Ph.D. Thesis, Western Michigan University, Kalamazoo,
MI, USA, 2015.
21. Yao, S.; Swetha, P.; Zhu, Y. Nanomaterial-Enabled wearable sensors for healthcare. Adv. Healthc. Mater. 2018,
7, 1700889. [CrossRef] [PubMed]
22. Nakata, S.; Arie, T.; Akita, S.; Takei, K. Wearable, flexible, and multifunctional healthcare device with an
ISFET chemical sensor for simultaneous sweat pH and skin temperature monitoring. ACS Sens. 2017, 2,
443–448. [CrossRef]
23. Martinez, M.M.; Nielsen, J.M.; VanArsdel, K.; Cacace, A.A. Wristband health tracker. U.S. Patent 29/500,837,
21 June 2016.
24. Farandos, N.M.; Yetisen, A.K.; Monteiro, M.J.; Lowe, C.R.; Yun, S.H. Contact lens sensors in ocular diagnostics.
Adv. Healthc. Mater. 2015, 4, 792–810. [CrossRef] [PubMed]
25. Abreu, M.M. Contact Lens for Collecting Tears and Detecting Analytes for Determining Health Status,
Ovulation Detection, and Diabetes Screening. U.S. Patent 7,809,417, 5 October 2010.
26. Kim, S.K.; Koo, J.; Lee, G.H.; Jeon, C.; Mok, J.W.; Mun, B.H.; Lee, K.J.; Kamrani, E.; Joo, C.K.; Shin, S.; et al.
Wireless smart contact lens for diabetic diagnosis and therapy. Sci. Adv. 2020, 6, eaba3252. [CrossRef]
[PubMed]
27. Wearables Market Trending Upward. Available online: https://www.printedelectronicsnow.com/issues/2019-
11-01/view_features/wearables-market-trending-upward/46378 (accessed on 12 September 2020).
28. Cheng, H.; Yi, N. Dissolvable tattoo sensors: From science fiction to a viable technology. Phys. Scr. 2016,
92, 013001. [CrossRef]
29. Liu, Y.; Wang, H.; Zhao, W.; Zhang, M.; Qin, H.; Xie, Y. Flexible, stretchable sensors for wearable health
monitoring: Sensing mechanisms, materials, fabrication strategies and features. Sensors 2018, 18, 645.
[CrossRef] [PubMed]
30. Shetti, N.P.; Mishra, A.; Basu, S.; Mascarenhas, R.J.; Kakarla, R.R.; Aminabhavi, T.M. Skin-Patchable Electrodes
for Biosensor Applications: A Review. ACS Biomater. Sci. Eng. 2020, 6, 1823–1835. [CrossRef]
31. Dinesh, M. Development of Fully Printed and Flexible Strain, Pressure and Electrochemical Sensors.
Master’s Thesis, Western Michigan University, Kalamazoo, MI, USA, 2016.
32. Suganuma, K. Introduction to Printed Electronics; Springer Science & Business Media: Berlin, Germany, 2014;
p. 74, ISBN 978-1-4614-9625-0.
33. Liao, Y.; Zhang, R.; Qian, J. Printed electronics based on inorganic conductive nanomaterials and their
applications in intelligent food packaging. RSC Adv. 2019, 9, 29154–29172. [CrossRef]
Biosensors 2020, 10, 199 18 of 24
34. Dahiya, A.S.; Shakthivel, D.; Kumaresan, Y.; Zumeit, A.; Christou, A.; Dahiya, R. High-performance printed
electronics based on inorganic semiconducting nano to chip scale structures. Nano Converg. 2020, 7, 1–25.
[CrossRef]
35. Reddy, A.S.G.; Narakathu, B.B.; Eshkeiti, A.; Bazuin, B.J.; Joyce, M.; Atashbar, M.Z. Fully printed organic
thin film transistors (OTFT) based flexible humidity sensors. In Proceedings of the IEEE Sensors Conference
Proceedings, Baltimore, MD, USA, 3–6 November 2013; pp. 1–4. [CrossRef]
36. Turkani, V.S.; Maddipatla, D.; Narakathu, B.B.; Bazuin, B.J.; Atashbar, M.Z. A carbon nanotube based NTC
thermistor using additive print manufacturing processes. Sens. Actuators A Phys. 2018, 279, 1–9. [CrossRef]
37. Ali, M.M.; Maddipatla, D.; Narakathu, B.B.; Chlaihawi, A.A.; Emamian, S.; Janabi, F.; Bazuin, B.J.;
Atashbar, M.Z. Printed strain sensor based on silver nanowire/silver flake composite on flexible and
stretchable TPU substrate. Sens. Actuators A Phys. 2018, 274, 109–115. [CrossRef]
38. A Wireless Sensing Platform for Every Surface—Boeing’s Condition Monitoring Sensor Array.
Available online: http://flex.semi.org/programs-catalog/flex-session-3-fhe-applications/wireless-sensing-
platform-every-surface%E2%80%94boeing%E2%80%99s-condition-monitoring-sensor-array (accessed on
12 September 2020).
39. Lim, S.; Joyce, M.; Fleming, P.D.; Aijazi, A.T.; Atashbar, M. Inkjet printing and sintering of nano-copper ink.
J. Imaging Sci. Technol. 2013, 57, 50506-1–50506-7. [CrossRef]
40. Tehrani, Z.; Thomas, D.J.; Korochkina, T.; Phillips, C.O.; Lupo, D.; Lehtimaki, S.; Omahony, J.; Gethin, D.T.
Large-area printed supercapacitor technology for low-cost domestic green energy storage. Energy 2017, 118,
1313–1321. [CrossRef]
41. Kang, J.S.; Kim, H.S.; Ryu, J.; Hahn, H.T.; Jang, S.; Joung, J.W. Inkjet printed electronics using copper
nanoparticle ink. J. Mater. Sci. Mater. Electron. 2010, 21, 1213–1220. [CrossRef]
42. Beduk, T.; Bihar, E.; Surya, S.G.; Castillo, A.N.; Inal, S.; Salama, K.N. A paper-based inkjet-printed PEDOT:
PSS/ZnO sol-gel hydrazine sensor. Sens. Actuators B Chem. 2020, 306, 127539. [CrossRef]
43. Arias, A.C.; MacKenzie, J.D.; McCulloch, I.; Rivnay, J.; Salleo, A. Materials and applications for large area
electronics: Solution-based approaches. Chem. Rev. 2010, 110, 3–24. [CrossRef] [PubMed]
44. Wang, X.; Liu, J. Recent advancements in liquid metal flexible printed electronics: Properties, technologies,
and applications. Micromachines 2016, 7, 206. [CrossRef]
45. Chang, W.Y.; Fang, T.H.; Lin, H.J.; Shen, Y.T.; Lin, Y.C. A large area flexible array sensors using screen printing
technology. J. Disp. Technol. 2009, 5, 178–183. [CrossRef]
46. Stringer, J.; Althagathi, T.M.; Tse, C.C.; Ta, V.D.; Shephard, J.D.; Esenturk, E.; Connaughton, C.; Wasley, T.J.;
Li, J.; Kay, R.W.; et al. Integration of additive manufacturing and inkjet printed electronics: A potential route
to parts with embedded multifunctionality. Manuf. Rev. 2016, 3, 12. [CrossRef]
47. Katerinopoulou, D.; Zalar, P.; Sweelssen, J.; Kiriakidis, G.; Rentrop, C.; Groen, P.; Gelinck, G.H.;
van den Brand, J.; Smits, E.C. Large-area all-printed temperature sensing surfaces using novel composite
thermistor materials. Adv. Electron. Mater. 2019, 5, 1800605. [CrossRef]
48. Fu, S.; Tao, J.; Wu, W.; Sun, J.; Li, F.; Li, J.; Huo, Z.; Xia, Z.; Bao, R.; Pan, C. Fabrication of large-area bimodal
sensors by all-inkjet-printing. Adv. Mater. Technol. 2019, 4, 1800703. [CrossRef]
49. Cui, Z. Printed Electronics: Materials, Technologies and Applications; John Wiley & Sons: Hoboken, NJ, USA, 2016.
50. Hoeng, F.; Denneulin, A.; Bras, J. Use of nanocellulose in printed electronics: A review. Nanoscale 2016, 8,
13131–13154. [CrossRef] [PubMed]
51. Caironi, M.; Gili, E.; Sakanoue, T.; Cheng, X.; Sirringhaus, H. High yield, single droplet electrode arrays for
nanoscale printed electronics. ACS Nano 2010, 4, 1451–1456. [CrossRef] [PubMed]
52. Lessing, J.; Glavan, A.C.; Walker, S.B.; Keplinger, C.; Lewis, J.A.; Whitesides, G.M. Inkjet Printing of
conductive inks with high lateral resolution on omniphobic “Rf paper” for paper-based electronics and
MEMS. Adv. Mater. 2014, 26, 4677–4682. [CrossRef] [PubMed]
53. Maddipatla, D.; Narakathu, B.B.; Ali, M.M.; Chlaihawi, A.A.; Atashbar, M.Z. Development of a novel carbon
nanotube based printed and flexible pressure sensor. In Proceedings of the 2017 IEEE Sensors Applications
Symposium (SAS), Glassboro, NJ, USA, 13–15 March 2017; pp. 1–4. [CrossRef]
54. Visakh, P.M.; Semkin, A.O. (Eds.) High Performance Polymers and Their Nanocomposites; John Wiley & Sons:
Hoboken, NJ, USA, 2018; ISBN 1119363888.
55. Sondhi, K.; Hwangbo, S.; Yoon, Y.K.; Nishida, T.; Fan, Z.H. Airbrushing and surface modification for
fabricating flexible electronics on polydimethylsiloxane. J. Micromech. Microeng. 2018, 28, 125014. [CrossRef]
Biosensors 2020, 10, 199 19 of 24
56. Li, C.Y.; Liao, Y.C. Adhesive stretchable printed conductive thin film patterns on PDMS surface with an
atmospheric plasma treatment. ACS Appl. Mater. Interfaces 2016, 8, 11868–11874. [CrossRef] [PubMed]
57. Agate, S.; Joyce, M.; Lucia, L.; Pal, L. Cellulose and nanocellulose-based flexible-hybrid printed electronics
and conductive composites—A review. Carbohydr. Polym. 2018, 198, 249–260. [CrossRef]
58. Sato, S.; Yamaguchi, T.; Shibata, K.; Nishi, T.; Moriyasu, K.; Harano, K.; Hokkirigawa, K. Dry sliding friction
and Wear behavior of thermoplastic polyurethane against abrasive paper. Biotribology 2020, 23, 100130.
[CrossRef]
59. Izdebska-Podsiadły, J.; Thomas, S. (Eds.) Printing on Polymers: Fundamentals and Applications; Elsevier:
Amsterdam, The Netherlands, 2015; ISBN 0323375006.
60. Kamyshny, A.; Magdassi, S. Conductive nanomaterials for printed electronics. Small 2014, 10, 3515–3535.
[CrossRef] [PubMed]
61. Junaidi, J.; Triyana, K.; Harsojo, H.; Suharyadi, E. High-performance silver nanowire film on flexible substrate
prepared by meyer-rod coating. Mater. Sci. Eng. 2017, 202, 012055. [CrossRef]
62. Marinho, B.; Ghislandi, M.; Tkalya, E.; Koning, C.E.; de With, G. Electrical conductivity of compacts of
graphene, multi-wall carbon nanotubes, carbon black, and graphite powder. Powder Technol. 2012, 221,
351–358. [CrossRef]
63. Tulliani, J.M.; Inserra, B.; Ziegler, D. Carbon-based materials for humidity sensing: A short review.
Micromachines 2019, 10, 232. [CrossRef]
64. Pajor-Swierzy, A.; Farraj, Y.; Kamyshny, A.; Magdassi, S. Effect of carboxylic acids on conductivity of metallic
films formed by inks based on copper@ silver core-shell particles. Colloids Surf. A Physicochem. Eng. Asp.
2017, 522, 320–327. [CrossRef]
65. Huang, Q.; Zhu, Y. Printing conductive nanomaterials for flexible and stretchable electronics: A review of
materials, processes, and applications. Adv. Mater. Technol. 2019, 4, 1800546. [CrossRef]
66. Altay, B.N.; Jourdan, J.; Turkani, V.S.; Dietsch, H.; Maddipatla, D.; Pekarovicova, A.; Fleming, P.D.;
Atashbar, M. Impact of substrate and process on the electrical performance of screen-printed nickel electrodes:
Fundamental mechanism of ink film roughness. ACS Appl. Energy Mater. 2018, 1, 7164–7173. [CrossRef]
67. Ahmad, M.; Malik, S.; Dewan, S.; Bose, A.K.; Maddipatla, D.; Narakathu, B.B.; Atashbar, M.Z.; Baghini, M.S.
An Auto-Calibrated Resistive Measurement System with Low Noise Instrumentation ASIC. IEEE J.
Solid-State Circuits 2020. [CrossRef]
68. Hu, G.; Kang, J.; Ng, L.W.; Zhu, X.; Howe, R.C.; Jones, C.G.; Hersam, M.C.; Hasan, T. Functional inks and
printing of two-dimensional materials. Chem. Soc. Rev. 2018, 47, 3265–3300. [CrossRef]
69. Huang, Q.; Zhu, Y. Gravure printing of water-based silver nanowire ink on plastic substrate for flexible
electronics. Sci. Rep. 2018, 8, 1–10. [CrossRef]
70. Ochoa, M.; Rahimi, R.; Zhou, J.; Jiang, H.; Yoon, C.K.; Maddipatla, D.; Narakathu, B.B.; Jain, V.; Oscai, M.M.;
Morken, T.J.; et al. Integrated sensing and delivery of oxygen for next-generation smart wound dressings.
Microsyst. Nanoeng. 2020, 6, 1–16. [CrossRef]
71. Tang, A.; Liu, Y.; Wang, Q.; Chen, R.; Liu, W.; Fang, Z.; Wang, L. A new photoelectric ink based on
nanocellulose/CdS quantum dots for screen-printing. Carbohydr. Polym. 2016, 148, 29–35. [CrossRef]
[PubMed]
72. Faddoul, R.; Reverdy-Bruas, N.; Blayo, A. Formulation and screen printing of water based conductive flake
silver pastes onto green ceramic tapes for electronic applications. Mater. Sci. Eng. B 2012, 177, 1053–1066.
[CrossRef]
73. Chen, X.; Jiang, H.; Hayes, R.A.; Li, X.; He, T.; Zhou, G. Screen printing insulator coatings for electrofluidic
display devices. Phys. Status Solidi A 2015, 212, 2023–2030. [CrossRef]
74. Schlisske, S.; Rosenauer, C.; Rödlmeier, T.; Giringer, K.; Michels, J.J.; Kremer, K.; Lemmer, U.; Morsbach, S.;
Daoulas, K.C.; Hernandez-Sosa, G. Ink Formulation for Printed Organic Electronics: Investigating Effects of
Aggregation on Structure and Rheology of Functional Inks Based on Conjugated Polymers in Mixed Solvents.
Adv. Mater. Technol. 2020, 2000335. [CrossRef]
75. Daalkhaijav, U.; Yirmibesoglu, O.D.; Walker, S.; Mengüç, Y. Rheological modification of liquid metal for
additive manufacturing of stretchable electronics. Adv. Mater. Technol. 2018, 3, 1700351. [CrossRef]
76. Morgan, M.L.; Curtis, D.J.; Deganello, D. Control of morphological and electrical properties of flexographic
printed electronics through tailored ink rheology. Org. Electron. 2019, 73, 212–218. [CrossRef]
Biosensors 2020, 10, 199 20 of 24
77. Irgens, F. Rheology and Non-Newtonian Fluids; Springer International Publishing: New York, NY, USA, 2014;
ISBN 978-3-319-01052-6. [CrossRef]
78. Alexander, D.E. Nature’s Machines: An Introduction to Organismal Biomechanics; Academic Press: Cambridge,
MA, USA, 2017. [CrossRef]
79. Khandavalli, S.; Rothstein, J.P. Ink transfer of non-Newtonian fluids from an idealized gravure cell: The effect
of shear and extensional deformation. J. Non-Newton. Fluid Mech. 2017, 243, 16–26. [CrossRef]
80. Ozkan, M.; Dimic-Misic, K.; Karakoc, A.; Hashmi, S.G.; Lund, P.; Maloney, T.; Paltakari, J. Rheological
characterization of liquid electrolytes for drop-on-demand inkjet printing. Org. Electron. 2016, 38, 307–315.
[CrossRef]
81. Derby, B. Inkjet printing of functional and structural materials: Fluid property requirements, feature stability,
and resolution. Annu. Rev. Mater. Res. 2020, 40, 395–414. [CrossRef]
82. Surface Tension and Water. Available online: https://www.usgs.gov/special-topic/water-science-school/
science/surface-tension-and-water?qt-science_center_objects=0#qt-science_center_objects (accessed on
12 September 2020).
83. Berry, J.D.; Neeson, M.J.; Dagastine, R.R.; Chan, D.Y.; Tabor, R.F. Measurement of surface and interfacial
tension using pendant drop tensiometry. J. Colloid Interface Sci. 2015, 454, 226–237. [CrossRef] [PubMed]
84. Chaudhuri, B. Biopolymers-graphene oxide nanoplatelets composites with enhanced conductivity and
biocompatibility suitable for tissue engineering applications. In Fullerens, Graphenes and Nanotubes;
William Andrew Publishing: Norwich, NY, USA, 2018; pp. 457–544.
85. Altay, B.N.; Ma, R.; Fleming, P.D.; Joyce, M.J.; Anand, A.; Chen, T.; Keskin, B.; Maddipatla, D.;
Turkani, V.S.; Kotkar, P.R.; et al. Surface Free Energy Estimation: A New Methodology for Solid Surfaces.
Adv. Mater. Interfaces 2020, 7, 1901570. [CrossRef]
86. Ali, S.; Maddipatla, D.; Narakathu, B.B.; Chlaihawi, A.A.; Emamian, S.; Janabi, F.; Bazuin, B.J.; Atashbar, M.Z.
Flexible capacitive pressure sensor based on pdms substrate and Ga–In liquid metal. IEEE Sens. J. 2018, 19,
97–104. [CrossRef]
87. Gerhard, C.; Roux, S.; Brückner, S.; Wieneke, S.; Viol, W. Low-temperature atmospheric pressure argon
plasma treatment and hybrid laser-plasma ablation of barite crown and heavy flint glass. Appl. Opt. 2012, 51,
3847–3852. [CrossRef] [PubMed]
88. Turkani, V.S.; Maddipatla, D.; Narakathu, B.B.; Saeed, T.S.; Obare, S.O.; Bazuin, B.J.; Atashbar, M.Z. A highly
sensitive printed humidity sensor based on a functionalized MWCNT/HEC composite for flexible electronics
application. Nanoscale Adv. 2019, 1, 2311–2322. [CrossRef]
89. Lawal, S.A.; Ndaliman, M.B. Surface Roughness Characteristics in Finish Electro-Discharge Machining Process;
Elsevier: Amsterdam, The Netherlands, 2017. [CrossRef]
90. Kipphan, H. Handbook of Print Media: Technologies and Production Methods; Springer: New York, NY, USA, 2001.
91. Wu, W. Inorganic nanomaterials for printed electronics: A review. Nanoscale 2017, 9, 7342–7372. [CrossRef]
92. Metters, J.P.; Kadara, R.O.; Banks, C.E. New directions in screen printed electroanalytical sensors: An overview
of recent developments. Analyst 2011, 136, 1067–1076. [CrossRef]
93. Eshkeiti, A.; Reddy, A.S.; Emamian, S.; Narakathu, B.B.; Joyce, M.; Joyce, M.; Fleming, P.D.; Bazuin, B.J.;
Atashbar, M.Z. Screen printing of multilayered hybrid printed circuit boards on different substrates.
IEEE Trans. Compon. Packag. Manuf. Technol. 2015, 5, 415–421. [CrossRef]
94. Cao, X.; Chen, H.; Gu, X.; Liu, B.; Wang, W.; Cao, Y.; Wu, F.; Zhou, C. Screen printing as a scalable and
low-cost approach for rigid and flexible thin-film transistors using separated carbon nanotubes. ACS Nano
2014, 8, 12769–12776. [CrossRef]
95. Avuthu, S.G.R.; Wabeke, J.T.; Narakathu, B.B.; Maddipatla, D.; Arachchilage, J.S.; Obare, S.O.; Atashbar, M.Z.
A screen printed phenanthroline-based flexible electrochemical sensor for selective detection of toxic heavy
metal ions. IEEE Sens. J. 2016, 16, 8678–8684. [CrossRef]
96. Narakathu, B.B.; Devadas, M.S.; Reddy, A.S.G.; Eshkeiti, A.; Moorthi, A.; Fernando, I.R.; Miller, B.P.;
Ramakrishna, G.; Sinn, E.; Joyce, M.; et al. Novel fully screen printed flexible electrochemical sensor for the
investigation of electron transfer between thiol functionalized viologen and gold clusters. Sens. Actuators
B Chem. 2013, 176, 768–774. [CrossRef]
Biosensors 2020, 10, 199 21 of 24
97. Avuthu, S.G.R.; Wabeke, J.T.; Narakathu, B.B.; Maddipatla, D.; Eshkeiti, A.; Emamian, S.; Chlaihawi, A.A.;
Joyce, M.; Obare, S.O.; Atashbar, M.Z. Development of screen printed electrochemical sensors for selective
detection of heavy metals. In Proceedings of the IEEE Sensors Conference Proceedings, Busan, Korea,
1–4 November 2015; pp. 1–4. [CrossRef]
98. Saeed, T.S.; Maddipatla, D.; Narakathu, B.B.; Albalawi, S.S.; Obare, S.O.; Atashbar, M.Z. Synthesis of a novel
hexaazatriphenylene derivative for the selective detection of copper ions in aqueous solution. RSC Adv.
2019, 9, 39824–39833. [CrossRef]
99. Maddipatla, D.; Saeed, T.S.; Narakathu, B.B.; Obare, S.O.; Atashbar, M.Z. Incorporating a Novel
Hexaazatriphenylene Derivative to a Flexible Screen-Printed Electrochemical Sensor for Copper Ion Detection
in Water Samples. IEEE Sens. J. 2020, 20, 12582–12591. [CrossRef]
100. Emamian, S.; Narakathu, B.B.; Chlaihawi, A.A.; Bazuin, B.J.; Atashbar, M.Z. Screen printing of flexible
piezoelectric based device on polyethylene terephthalate (PET) and paper for touch and force sensing
applications. Sens. Actuators A Phys. 2017, 263, 639–647. [CrossRef]
101. Turkani, V.S.; Maddipatla, D.; Narakathu, B.B.; Altay, B.N.; Fleming, P.D.; Bazuin, B.J.; Atashbar, M.Z. Nickel
Based RTD Fabricated via Additive Screen Printing Process for Flexible Electronics. IEEE Access 2019, 7,
37518–37527. [CrossRef]
102. Yoon, S.; Kim, H.K. Cost-effective stretchable Ag nanoparticles electrodes fabrication by screen printing for
wearable strain sensors. Surf. Coat. Technol. 2020, 384, 125308. [CrossRef]
103. Bose, A.K.; Zhang, X.; Maddipatla, D.; Masihi, S.; Panahi, M.; Narakathu, B.B.; Bazuin, B.J.; Atashbar, M.Z.
Highly Sensitive Screen Printed Strain Gauge for Micro-Strain Detection. In Proceedings of the IEEE
International Conference on Flexible and Printable Sensors and Systems (FLEPS), Glasgow, UK, 8–10 July 2019;
pp. 1–3. [CrossRef]
104. Feng, X.; Yang, B.D.; Liu, Y.; Wang, Y.; Dagdeviren, C.; Liu, Z.; Carlson, A.; Li, J.; Huang, Y.; Rogers, J.A.
Stretchable ferroelectric nanoribbons with wavy configurations on elastomeric substrates. ACS Nano 2011, 5,
3326–3332. [CrossRef]
105. Tian, B.; Yao, W.; Zeng, P.; Li, X.; Wang, H.; Liu, L.; Feng, Y.; Luo, C.; Wu, W. All-printed, low-cost, tunable
sensing range strain sensors based on Ag nanodendrite conductive inks for wearable electronics. J. Mater.
Chem. C 2019, 7, 809–818. [CrossRef]
106. Bose, A.K.; Zhang, X.; Maddipatla, D.; Masihi, S.; Panahi, M.; Narakathu, B.B.; Bazuin, B.J.; Williams, J.D.;
Mitchell, M.F.; Atashbar, M.Z. Screen-Printed Strain Gauge for Micro-Strain Detection Applications.
IEEE Sens. J. 2020, 20, 12652–12660. [CrossRef]
107. Cao, R.; Pu, X.; Du, X.; Yang, W.; Wang, J.; Guo, H.; Zhao, S.; Yuan, Z.; Zhang, C.; Li, C.; et al. Screen-printed
washable electronic textiles as self-powered touch/gesture tribo-sensors for intelligent human–machine
interaction. ACS Nano 2018, 12, 5190–5196. [CrossRef]
108. Cinti, S.; Arduini, F. Graphene-based screen-printed electrochemical (bio) sensors and their applications:
Efforts and criticisms. Biosens. Bioelectron. 2017, 89, 107–122. [CrossRef] [PubMed]
109. Maddipatla, D.; Narakathu, B.B.; Bazuin, B.J.; Atashbar, M.Z. Development of a printed impedance based
electrochemical sensor on paper substrate. In Proceedings of the IEEE Sensors Conference Proceedings,
Orlando, FL, USA, 30 October–3 November 2016; pp. 1–3. [CrossRef]
110. Eggenhuisen, T.M.; Galagan, Y.; Biezemans, A.F.K.V.; Slaats, T.M.W.L.; Voorthuijzen, W.P.; Kommeren, S.;
Shanmugam, S.; Teunissen, J.P.; Hadipour, A.; Verhees, W.J.H.; et al. High efficiency, fully inkjet printed
organic solar cells with freedom of design. J. Mater. Chem. A 2015, 3, 7255–7262. [CrossRef]
111. Corzo, D.; Almasabi, K.; Bihar, E.; Macphee, S.; Rosas-Villalva, D.; Gasparini, N.; Inal, S.; Baran, D. Digital
Inkjet Printing of High-Efficiency Large-Area Nonfullerene Organic Solar Cells. Adv. Mater. Technol. 2019,
4, 1900040. [CrossRef]
112. Focus Label Machinery Launches Digital Inkjet Press. Available online: https://www.labelsandlabeling.com/
news/new-products/focus-label-machinery-launches-digital-inkjet-press (accessed on 15 September 2020).
113. Ochoa, M.; Rahimi, R.; Zhou, J.; Jiang, H.; Yoon, C.K.; Oscai, M.; Jain, V.; Morken, T.; Oliveira, R.H.;
Maddipatla, D.; et al. A manufacturable smart dressing with oxygen delivery and sensing capability for
chronic wound management. Micro Nanotechnol. Sens. Syst. Appl. 2018, 10639, 106391C. [CrossRef]
114. Maddipatla, D.; Narakathu, B.B.; Ochoa, M.; Rahimi, R.; Zhou, J.; Yoon, C.K.; Jiang, H.; Al-Zubaidi, H.;
Obare, S.O.; Zieger, M.A.; et al. Rapid prototyping of a novel and flexible paper based oxygen sensing patch
via additive inkjet printing process. RSC Adv. 2019, 9, 22695–22704. [CrossRef]
Biosensors 2020, 10, 199 22 of 24
136. Bariya, M.; Shahpar, Z.; Park, H.; Sun, J.; Jung, Y.; Gao, W.; Nyein, H.Y.Y.; Liaw, T.S.; Tai, L.C.; Ngo, Q.P.; et al.
Roll-to-roll gravure printed electrochemical sensors for wearable and medical devices. ACS Nano 2018, 12,
6978–6987. [CrossRef] [PubMed]
137. Lau, P.H.; Takei, K.; Wang, C.; Ju, Y.; Kim, J.; Yu, Z.; Takahashi, T.; Cho, G.; Javey, A. Fully printed, high
performance carbon nanotube thin-film transistors on flexible substrates. Nano Lett. 2013, 13, 3864–3869.
[CrossRef] [PubMed]
138. Shrestha, S.; Yerramilli, R.; Karmakar, N.C. Microwave performance of flexo-printed chipless RFID tags.
Flex. Print. Electron. 2019, 4, 045003. [CrossRef]
139. Gordon, S.E.; Dorfman, J.R.; Kirk, D.; Adams, K. Advances in Conductive Inks across Multiple Applications
and Deposition Platforms. DuPont Microcircuit Materials. In Proceedings of the IEEE Photonics Conference,
Arlington, VA, USA, 9–13 October 2011; Available online: https://smtnet.com/library/files/upload/Conductive-
Inks-Advances.pdf (accessed on 5 September 2020).
140. Benson, J.; Fung, C.M.; Lloyd, J.S.; Deganello, D.; Smith, N.A.; Teng, K.S. Direct patterning of gold
nanoparticles using flexographic printing for biosensing applications. Nanoscale Res. Lett. 2015, 10, 1–8.
[CrossRef]
141. Fung, C.M.; Lloyd, J.S.; Samavat, S.; Deganello, D.; Teng, K.S. Facile fabrication of electrochemical ZnO
nanowire glucose biosensor using roll to roll printing technique. Sens. Actuators B Chem. 2017, 247, 807–813.
[CrossRef]
142. Tian, J.; Arbatan, T.; Li, X.; Shen, W. Liquid marble for gas sensing. Chem. Commun. 2010, 46, 4734–4736.
[CrossRef]
143. Hoekstra, D.C.; Nickmans, K.; Lub, J.; Debije, M.G.; Schenning, A.P. Air-curable, high-resolution patternable
oxetane-based liquid crystalline photonic films via flexographic printing. ACS Appl. Mater. Interfaces 2019,
11, 7423–7430. [CrossRef]
144. Higuchi, K.; Kishimoto, S.; Nakajima, Y.; Tomura, T.; Takesue, M.; Hata, K.; Kauppinen, E.I.; Ohno, Y.
High-mobility, flexible carbon nanotube thin-film transistors fabricated by transfer and high-speed
flexographic printing techniques. Appl. Phys. Express 2013, 6, 085101. [CrossRef]
145. Hübler, A.C.; Bellmann, M.; Schmidt, G.C.; Zimmermann, S.; Gerlach, A.; Haentjes, C. Fully mass printed
loudspeakers on paper. Org. Electron. 2012, 13, 2290–2295. [CrossRef]
146. Maddipatla, D.; Narakathu, B.B.; Avuthu, S.G.R.; Emamian, S.; Eshkeiti, A.; Chlaihawi, A.A.; Bazuin, B.J.;
Joyce, M.K.; Barrett, C.W.; Atashbar, M.Z. A novel flexographic printed strain gauge on paper platform.
In Proceedings of the IEEE Sensors Conference Proceedings, Busan, Korea, 1–4 November 2015; pp. 1–4.
[CrossRef]
147. Joannou, G. The Printing Ink Manual—Screen Inks; Springer: New York, NY, USA, 1988; pp. 481–514. [CrossRef]
148. Controlling the Variables That Affect Your Screen Printing Ink Deposit. Available online: https://anatol.com/
controlling-the-variables-that-affect-your-screen-printing-ink-deposit/ (accessed on 5 September 2020).
149. Li, Y.; Dahhan, O.; Filipe, C.D.; Brennan, J.D.; Pelton, R.H. Deposited Nanoparticles Can Promote Air
Clogging of Piezoelectric Inkjet Printhead Nozzles. Langmuir 2019, 35, 5517–5524. [CrossRef] [PubMed]
150. Martin, G.D.; Hoath, S.D.; Hutchings, I.M. March. Inkjet printing-the physics of manipulating liquid jets and
drops. J. Phys. Conf. Ser. 2008, 105, 012001. [CrossRef]
151. Hill, R. Gravure & Its Role in Printed Electronics. Gravure, Association of the Americas. 2006. Available
online: https://gaa.org/gravure-its-role-in-printed-electronics/#:~{}:text=Disadvantages%20of%20Gravure%
20for%20Printing,thoroughly%20(Birkenshaw%2C%202004) (accessed on 5 September 2020).
152. Understanding Common Flexo Printing Defects: Mottled Print. Available online: https://blog.luminite.com/
blog/flexo-printing-defects-mottled-image (accessed on 5 September 2020).
153. NextFlex. Available online: https://www.manufacturingusa.com/institutes/nextflex (accessed on 5 September 2020).
154. Welcome to NextFlex. Available online: https://www.nextflex.us/ (accessed on 5 September 2020).
155. HI-RESPONSE. Available online: http://www.hi-responseh2020.eu/index.html (accessed on 9 November 2020).
156. MADRAS. Available online: https://madras-project.eu/ (accessed on 9 November 2020).
157. Su, Y.; Ma, C.; Chen, J.; Wu, H.; Luo, W.; Peng, Y.; Luo, Z.; Li, L.; Tan, Y.; Omisore, O.M.; et al. Printable,
Highly Sensitive Flexible Temperature Sensors for Human Body Temperature Monitoring: A Review.
Nanoscale Res. Lett. 2020, 15, 1–34. [CrossRef] [PubMed]
158. Elgeneidy, K.; Neumann, G.; Jackson, M.; Lohse, N. Directly Printable Flexible Strain Sensors for Bending
and Contact Feedback of Soft Actuators. Front. Robot. AI 2018, 5, 2. [CrossRef]
Biosensors 2020, 10, 199 24 of 24
159. Senthil Kumar, K.; Chen, P.Y.; Ren, H. A Review of Printable Flexible and Stretchable Tactile Sensors. Research
2019, 2019, 1–32. [CrossRef] [PubMed]
160. Windmiller, J.R.; Wang, J. Wearable Electrochemical Sensors and Biosensors: A Review. Electroanalysis 2013,
25, 29–46. [CrossRef]
Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional
affiliations.
© 2020 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access
article distributed under the terms and conditions of the Creative Commons Attribution
(CC BY) license (http://creativecommons.org/licenses/by/4.0/).