BIOSENSORS

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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].

Biosensors 2020, 10, 199; doi:10.3390/bios10120199 www.mdpi.com/journal/biosensors


Biosensors 2020, 10, 199 2 of 24

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. Materials and Characterization Methods

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

Table 1. Specifications of various substrates employed in printed electronics (PE).

Substrate PET PI PEN TPU Paper PDMS


Classification Thermoplastic Polymer Cellulose Fibers Silicone Elastomer
Thickness (µm) 13–356 25–125 12.5–250 25–500 20–250 125–4775
Roughness (µm) ≈0.04 ≈0.07 ≈0.025 0.02–5 ~0.24
Tg (◦ C) 81–150 360–410 120–200 ~80 145–150
Density (g/cc) 1.38 1.42 1.33 1.32 0.6–1.0 0.97
Young’s Modulus
2–3.2 2.76 2.2–3.0 2.41 0.5–3.5 0.57–3.7
(GPa)
Folding Endurance
>800 5000–285,000 >1000 2,000,000 -
(Cycles)
Pros: Transparency, Pros: High Thermal, Pros: Transparency, Pros: Stretchable Pros: Cheap/Low Pros: Biodegradable,
Smoothness, Mechanical and Relatively Higher Unlike Other Plastic Cost, Ecofriendly, Non-Toxic, High
Economical Chemical Resistance Thermal and Polymers, Mechanical Available in Stretchability
Compared to Other Mechanical Stability and Chemical Abundance
Thermoplastic than PET Resistance, Less Gas
Polymers Permeability than
PET
Cons: Low Tg Cons: Cons: High Cost than Cons: Relatively High Cons: Low Cons: Low
Comments (Pros,
Non-Transparent, PET, Not as Good as Cost Mechanical and Mechanical and
Cons, Applications)
Relatively High Cost PI in Terms of all Chemical Resistance Chemical Resistance,
Properties Except Hydrophobic Surface
Cost (Low Surface Energy)
Applications: Optical, Applications: Applications: Flexible Applications: Wearable Applications: Applications: Wearable
Simple Printed Electrochemical Heaters, Electronics Disposable Devices and Biomedical
Circuitry, Sensing, TFTs, Opto-Electronic and Sensors Devices Including
Occupant/Pressure Flexible PCBs Sensors, Highly Used Microfluidics and
Sensors in Packaging as Sensors
Labels and Laminates,
Printed Circuits, and
Optical Displays
Biosensors 2020, 10, 199 5 of 24

Table 2. Different components present in the ink system.

Ink System Components (wt. %)


Printing Process Functional Element Binder Solvent Additives
Screen 35–55 30–20 30–20 1–5
Inkjet 5–10 5–20 65–95 1–5
Flexo 12–17 40–45 25–45 1–5
Gravure 12–17 20–35 60–65 1–2

2.3. Ink and Substrate Characterizations


The physical properties of the ink such as viscosity, surface tension, wetting characteristics,
and density are crucial to consider for obtaining a better print quality [70–73]. These properties of
the ink depend on the composition of the ink system components. Therefore, understanding these
properties and measuring them as part of pre-print characterization can significantly impact the output
quality of the printing processes.

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].

2.3.2. Surface Tension


Surface tension is the property of a fluid’s interface and is defined as the elastic tendency of
particles on the surface of the fluids resulting in the minimum possible surface area [82]. Surface tension
is an important property that markedly influences many ecosystems. In other words, surface tension
is described as the work required for disturbing the droplet shape of the fluid with intermolecular
forces that holds the fluid together at any air or liquid interface, as shown in Figure 1a. It is work done
per unit length, and the units are usually in dynes/cm or milli-newton/m (mN/m) [59]. The surface
tension of any ink system depends on the solvents used in it and can be altered by adding a very small
quantity of polar or non-polar surfactants to the ink system. There are many methods to measure the
surface tension in the liquids, but the pendant drop method is typically used to obtain the surface
particles on the surface of the fluids resulting in the minimum possible surface area [82]. Surface
tension is an important property that markedly influences many ecosystems. In other words, surface
tension is described as the work required for disturbing the droplet shape of the fluid with
intermolecular forces that holds the fluid together at any air or liquid interface, as shown in Figure
1a. It is work done per unit length, and the units are usually in dynes/cm or milli-newton/m (mN/m)
Biosensors The10,
[59].2020, 199 tension of any ink system depends on the solvents used in it and can be altered 6by
surface of 24
adding a very small quantity of polar or non-polar surfactants to the ink system. There are many
methods to measure the surface tension in the liquids, but the pendant drop method is typically used
tension which depends on analyzing the shape of the liquid droplet, in its biggest volume before it
to obtain the surface tension which depends on analyzing the shape of the liquid droplet, in its biggest
falls volume
down on the surface
before of theon
it falls down substrate [59,83].
the surface of the substrate [59,83].

(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.

2.3.3. Contact Angle and Surface Energy


The contact angle is often defined as the angle at which a liquid/vapor interface meets the solid
surface (substrate) [84]. The contact angle is specific for any given system and is measured using a
goniometer [59,66]. Contact angle measurement provides information about ink-surface interactions
(the behavior of the ink droplet at the substrate surface) and its wetting behavior. For example, if an ink
droplet does not spread well and forms a high contact angle (≥90◦ ), this implies that the ink-surface
interaction has poor wetting property (Figure 1b), and it is not desirable for printing applications. On the
other hand, printing applications require good wetting property (contact angle < 90◦ ). The contact
angle depends on several factors such as surface roughness, ink formulation, solvent properties, surface
energy, pre/post treatments (UV, plasma), and processing temperatures [59]. The goniometer helps to
determine the contact angle and the spreading of the fluid on the surface of the substrate.
Surface energy is measured for solid materials (substrates) and is defined as the amount of
intermolecular forces available at the surface of a material [85]. These forces can be exerted on to a
fluid droplet to disrupt its interfacial bonds. Typically, surface energy of a substrate is measured using
Owens and Wendt method (and new method: Altay–Ma–Fleming Method) and quantified in dynes/cm
or mN/m [85]. Techniques such as corona, UV ozone, sintering, plasma, and laser treatments are
employed to modify the surface energy of the substrates [59,86,87]. In printed electronics, the degree
of wetting, spreading, and adhesion of a deposited ink mainly depends on the surface energy of the
substrate and the surface tension of the liquid. In PE, it is always desirable to have the surface energy of
the substrate at least above 7–10 dynes/cm compared to surface tension of the ink to get good wetting
and adhesion characteristics [36,88].

2.3.4. Surface Characterization Methods


Surface characterization is the study of the surface characteristics/properties of a solid material
(e.g., substrates) [89]. In many applications, certain surface properties of the material such as roughness
are crucial. These properties can easily be altered through interaction with the open environment
due to physically or chemically adsorbed substances from gases, hydrocarbons, and water vapor [59].
Surface roughness has great influences on various other surface properties such as surface area, surface
energy, electrical resistance, and thermal conductivity. Therefore, depending on the application needs,
necessary modifications can be done to change roughness in order to achieve desirable changes
in other surface properties. In PE, various applications require substrates with different surface
properties. Before considering a material as a substrate, knowledge about its surface properties such as
roughness, micro-mechanical properties, and thickness is of utmost importance to achieve a fine print
quality. There are various surface characterization methods available to measure these parameters.
Biosensors 2020, 10, 199 7 of 24

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.

3. Printing Processes and Applications


The printing processes are classified into impact and non-impact printing processes. In the
impact printing process, the information on the printing plate/mask (information carrying medium)
corresponding to image elements (allowing ink transfer) and non-image elements (no transfer of
ink) is created on the substrate by the transfer of ink from plate to the surface of the substrate [90].
Screen, gravure, and flexography printing processes are classified as impact printing processes and
require a printing plate or a fixed image carrier for information transfer to substrate. On the other
hand, the non-impact printing (NIP) processes such as inkjet printing create/transfers information
on to the substrate digitally and do not require any printing plate or physical information carrying
medium [59,90,91]. Even though the NIP processes seem attractive compared to impact printing
processes, each printing method has its own advantages and provides a specific printed feature size.
The widely used printing techniques that are employed for the development of printed electronics
are screen, inkjet, flexographic, and gravure printing. Each printing process requires a particular set
of ink properties and results in specific printed features as shown in Table 3 [59,68]. Screen printing
requires very high viscosity inks with high functional element solid content and has been used for
depositing thick film layers with high repeatability. On the other hand, inkjet printing requires very
low viscosity inks and is being used for obtaining thin film layers with high resolution. Similarly,
flexography and gravure printing require medium viscosity inks and are completely compatible for
roll-to-roll (R2R) high volume production. For example, if the desired thickness of the printed film for
a particular application is 20 µm and the viscosity of the available ink system is 30 Pa.s, then the screen
printing process can be employed.

Table 3. Specifications of printing techniques employed in printed electronics.

Printing Film Thickness Printing Speed Resolution Viscosity


Image Carrier
Process (µm) (m/min) (µm) (Pa.s.)
Screen Stencil 3–60 0.6–100 30 0.5–60
Inkjet Digital 0.01–0.5 0.02–5 20 0.001–0.1
Flexo Polymer Plates 0.17–8 5–180 15 0.01–0.8
Gravure Engraved Cylinder 0.02–12 8–100 15 0.01–1.1

3.1. Screen Printing


Screen printing is a technique in which a paste-like material (ink) is transferred onto the substrate.
Screen printing is typically done either by hand or using a semi or fully automated system. The screen
printer consists of a squeegee, stencil, and a screen with the design on it (Figure 2a) [59,90]. Typically,
screen fibers are made of plastic, natural silk, or metal fibers, and the squeeze is made of rubber.
A section in the screen will be imposed by the design of the desired print and the ink is allowed to pass
through it, and the desired design is created on the substrate being used. The ink is transferred either
by pushing or forcing the ink by squeezing through the screen, and thus, this printing process is also
referred as push through process. The print quality mainly depends on the mesh count, wire diameter,
emulsion thickness, off-set height, and deflection angle of the screen. The screen-printing technique
has the capability to print electronic devices at a low cost, with very little or no material wastage
and provides an end product that can be extremely flexible [91,92]. With screen printing capabilities
including R2R manufacturing and processing at ambient conditions, it is possible to fabricate a large
number of printed devices in a relatively short period of time.
Biosensors 2020, 10, 199 8 of 24

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

(a) (b) (c)

(d) (e) (f) (g)


10 µm
≈17µm Ni
Kapton

(h) (i) (j) (k)

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;
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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.

3.2. Inkjet Printing


Inkjet printing is a non-impact printing method (NIP), and it uses a digital image signal
Biosensors 2020, 10, x; doi: FOR PEER REVIEW www.mdpi.com/journal/biosensors
to print the design by propelling ink droplets onto the substrate instead of any physical image
carriers [59,90]. Typically, in inkjet printing, the inks will be in a liquid state with low viscosities and
can be directly printed onto the substrate. Inkjet printing is classified into continuous inkjet printing
and drop-on-demand (DOD) inkjet printing. In continuous Inkjet printing, a continuous flow of
ink droplets is controlled electronically by a voltage source. Some of the ink droplets are subjected
to electrostatic charge and are deflected to get a negative print by electrostatic deflectors while the
uncharged drops are used to print the desired image onto the substrate. Thermal inkjet printers are very
popular in graphic printing and packaging industries. In a DOD-based inkjet printing, the ink droplets
are created only if it is required by the image signal to get the desired print [59,90]. The droplets are
formed either by using thermal or piezoelectric techniques as shown in Figure 3a. In thermal inkjet
printers, the ink droplets are forced or impelled out of the cartridge nozzle by a vapor bubble formed
because of the vaporization of ink liquid. In piezoelectric inkjet printers, the volume of the cartridge
Biosensors 2020, 10, 199 10 of 24

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)

(e) (f) (g) (h)

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

3.3. Gravure Printing


Gravure printing is an impact-based printing technique that provides economical production with
fast outputs along with high-quality printing. It uses low viscosity inks and is known for its robustness.
The image carrier cylinder (gravure cylinder), doctor blade, ink reservoir, and the impression cylinder
are some of the main components of the gravure printer as shown in Figure 4a [59,90]. Typically,
the impression cylinder is made of rubber, the gravure cylinder is made of copper coated steel, and the
doctor blade is manufactured with steel. In gravure printing, the image of the desired design is
engraved on the surface of the gravure cylinder. The entire gravure cylinder is flooded by ink from the
ink reservoir, and the extra ink is wiped off from the cylinder with the doctor blade prior to printing.
The ink is transferred onto the substrate from the gravure cylinder with high pressures, and the
substrate movement is controlled by the impression cylinder.
Antennas, SERS substrates, TFTs, electrochemical sensors, pressure sensors and many more
devices has been realized using gravure printing process [127–130]. For example, Maddipatla et al.
fabricated wrinkle-structure-based SERS substrate for the detection of illicit drugs such as cocaine
(Figure 4b) [131]. The wrinkle structures were created by subjecting the TPU substrate under varying
strains (25%, 50%, 75%, and 100%) and printing Ag ink with 150 nm particle size on stretched TPU
substrate using gravure printing process. Enhanced Raman signal intensity of cocaine (enhancement
factor of 6) was obtained due to the generation of larger electromagnetic fields. This was attributed to
the increase in the number and depth of hotspots caused by wrinkle patterned structures. In addition,
Zhu et al. fabricated for the first time a paper-based RFID antenna using gravure printing process
(Figure 4c) [132]. In this work, they prepared a stable transparent nanopaper by treating nanocellulose
fiber with glutaraldehyde treatment and hydrochloric (HCl) and UHF RFID antenna tag “squiggle”
was developed by depositing water-based Ag ink on the nanopaper using gravure printing process.
Insertion losses of −37.9 and −38.85 dB were obtained at the maximum gain of 683.75 MHz for the
100 lpi and 120 lpi printed antennas, respectively.
Dr. Atashbar and Dr. Joyce research groups from Western Michigan University were the first
to demonstrate large scale R2R fabrication of printed circuits and antenna structures using gravure
printing on both PET and paper substrates using conductive Ag ink in 2012 (Figure 4d) [133–135].
Further, Bariya et al. fabricated various electrochemical sensors on a PET roll for detecting ions,
metabolites, heavy metals, and other small molecules (Figure 4e) [136]. The sensors comprised
of carbon as working and counter electrode, Ag as reference electrode, and polyethylene resin as
encapsulant. To demonstrate the functionality of the printed electrodes, various sensing layers that
can selectively detect pH, sodium, potassium, glucose, and caffeine were deposited on the printed
arrays. Lau et al. developed fully printed CNT-based high performance TFT arrays using gravure
printing process (Figure 4f) [137]. Ag nanoparticle-based ink was gravure printed as source, drain,
and gate electrodes on SWCNT coated PET substrate. Then the insulator was also gravure printed using
barium titanate nanoparticles. The top gated fully oriented TFT exhibited excellent performance with
a mobility of ~9 cm2 /(V s), on/off current ratio of 105 and features minimal hysteresis, high flexibility,
and operational stability.
Biosensors 2020, 10, 199 13 of 24
Biosensors 2020, 10, x FOR PEER REVIEW 3 of 4

(a)

12 mm

(c) (b)

(d) (e) (f)


Figure 4. (a) Schematic of gravure printing process; (b) wrinkle-structure-based SERS substrate
withFigure
SEM4.micrographs
(a) Schematicshowing
of gravurethe
printing
plain process; (b) wrinkle-structure-based
and wrinkle SERS substrate
structures on stretchable with
thermoplastic
SEM micrographs
polyurethane showing
(TPU) substrate, the plain
Reprinted from and
[131] wrinkle structures
with permission fromon stretchable
Elsevier; thermoplastic
(c) stable transparent
polyurethane (TPU) substrate, Reprinted from [131] with permission from Elsevier;
nanopaper-based RFID antenna [132], Republished with Permission of RSC Pub; (d) R2R manufacturing (c) stable
of large area printed circuits and antenna structures; (e) electrochemical sensors on a PET(d)
transparent nanopaper-based RFID antenna [132], Republished with Permission of RSC Pub; rollR2R
for
manufacturing of large area printed circuits and antenna structures; (e) electrochemical
detecting ions, metabolites, heavy metals, and other small molecules, Reprinted with permission sensors on a
PET roll for detecting ions, metabolites, heavy metals, and other small molecules, Reprinted with
from [136], © American Chemical Society; (f) fully printed CNT-based high performance TFT arrays,
permission from [136], © American Chemical Society; (f) fully printed CNT-based high performance
Reprinted with permission from [137], © American Chemical Society.
TFT arrays, Reprinted with permission from [137], © American Chemical Society.
3.4. Flexographic Printing
Flexographic printing is a well-established R2R high throughput rotational printing method. It is
an indirect impact-based printing technique that can provide a wide range of ink thicknesses with the
same resolution. The main parts of the flexographic printer are anilox roller, an impression cylinder,
doctor blade, and the ink reservoir (Figure 5a) [59,90]. Anilox roller (a steel cylinder), which has finely
engraved cells on its surface made of chromium or ceramics, collects the specific amount of ink from
the ink reservoir. Then, the collected ink is transferred onto the elevated structures of the printing
plate. With the help of the plate cylinder, the ink on the printing plate is transferred on to the substrate.
It is capable of addressing problems such as contact finger geometry as well as production line output.
In addition, flexography has high speed R2R printing capability (up to 100 m per minute) when
compared to inkjet and screen printing [138,139]. Flexography printing is a well matured printing
technique in graphic printing and packaging industries. However, the implementation of flexographic
printing in FHE is not yet explored enough due to the limitations in research and commercial availability
Biosensors 2020, 10, 199 14 of 24

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)

(e) (f) (g)

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,
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with permission from©[143],
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Chemical
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(e) high (e) high
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CNT-based TFTs on PEN TFTs on PEN(15
substrate substrate
× 15 cm(15 × 15 cm2) (2013)
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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.

4. Conclusions and Outlook


The development of FHE-based devices using various additive printing processes is growing
exponentially due to obvious reasons—rapid-large area fabrication, cost efficiency, thin and light weight
devices. In this paper, the significance of printed electronics and the parameters to be considered
prior to printing and to be measured post-printing along with the numerous prototype devices
developed using each printing process is presented. There are still a few more scientific challenges that
need to be addressed to effectively perform research and adopt printing technologies for developing
FHE-based devices. For example, the screen-printing process provides high wet film thickness when
compared to other printing processes resulting in high spreading of ink and low resolution if not
cured instantly [59]. In addition, the ink will be exposed to atmosphere for long times while printing,
leading to solvent evaporation and deterioration of the mesh quality [59,147,148]. In inkjet printing,
developing inks for proper jetting of droplets in a specified area and cleaning cycles is challenging due
to the rate of evaporation of solvents and agglomeration of active particles, which leads to clogging
of nozzles [149,150]. In addition, the one-time use cartridges are expensive and, due to the limited
number of nozzles and slow speed of inkjet printing process (to avoid the deflections in the droplets
during the time of flight), the throughput/yield rate is relatively low when compared to other printing
processes [149,150].
In gravure printing, the gravure cylinder with pattern engravings is relatively expensive,
and during the printing process, a tiny portion of the ink gets clogged or remains in the cells
(etched walls) of the cylinder and dries out impacting the quality of the subsequent prints [151]. In both
flexography and gravure, the availability of functional inks is very low. Both of the printing processes
are well established in graphic printing industries and meant for continuous large-scale production.
To develop inks compatible for these two processes requires large volumes of functional materials
during the research phase with associated high costs. Due to these reasons, the research activities for
these two processes are still less when compared to screen and inkjet (requires a lower quantity of inks).
In addition, the outer edges of printed patterns in flexography typically suffer from squashed-ink
appearance due to numerous reasons (insufficient ink volumes, inappropriate anilox roller volume,
ink drying, viscosity, speed of machine) [59,152].
Due to these unresolved issues in printing, there are huge variations in the fabrication of FHE
devices (both device-to-device and batch-to-batch) leading to unreliable and unstable performance.
In addition, the variations in the environmental conditions including temperature and humidity
Biosensors 2020, 10, 199 16 of 24

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.

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