Journal of Energy Chemistry 63 (2021) 498–513

Contents lists available at ScienceDirect

Journal of Energy Chemistry

journal homepage: www.elsevier.com/locate/jechem

Ink formulation, scalable applications and challenging perspectives of

screen printing for emerging printed microelectronics
Ying Zhang a,d,1, Yuanyuan Zhu a,1, Shuanghao Zheng a,b, Liangzhu Zhang a, Xiaoyu Shi a, Jian He c,
Xiujian Chou c, Zhong-Shuai Wu a,b,⇑
a
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, Liaoning, China
b
Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, Liaoning, China
c
School of Instrument and Electronics, North University of China, Taiyuan 030051, Shanxi, China
d
University of Chinese Academy of Sciences, 19 A Yuquan Road, Beijing 100049, China

a r t i c l e i n f o a b s t r a c t

Article history: Screen printing is regarded as a highly competitive manufacture technology for scalable and fast fabrica-
Received 17 May 2021 tion of printed microelectronics, owing to its advanced merits of low-cost, facile operability and scalability.
Revised 5 August 2021 However, its large-scale application in printed microelectronics is still limited by screen printing functional
Accepted 6 August 2021
ink. In this review, we summarize the recent advances of ink formation, typical scalable applications, and
Available online 14 August 2021
challenging perspectives of screen printing for emerging printed microelectronics. Firstly, we introduce the
major mechanism of screen printing and the formation of different organic- and aqueous-based inks by
Keywords:
various solvents and binders. Next, we review the most widely used applications of screen printing tech-
Screen printing
Ink
nique in micro-batteries, micro-supercapacitors and micro-sensors, demonstrative of wide applicability.
Micro-batteries Finally, the perspectives and future challenges in the sight of screen printing are briefly discussed.
Micro-supercapacitors Ó 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published
Micro-sensors by ELSEVIER B.V. and Science Press. All rights reserved.

1. Introduction scale personalized ink-jet printer. Similarly, transfer printing could

The rapid advancement on smart wearable and integrated elec-
tronics has largely stimulated the ever-increasing demand of
printed microelectronics with light weight, high performance and
outstanding mechanical flexibility [1–4]. Therefore, the printed
microelectronics, such as micro-batteries (MBs), micro-
supercapacitors (MSCs) and micro-sensors, required easy integra-
tion, high flexibility and ability to customize novel designs for
specific applications [5]. For realizing the demand of flexible
printed electronics, various printing technologies, such as screen
printing [6–8], spray coating [9,10], inkjet printing [11–14], trans-
fer printing [15,16], 3D printing [17–20], and 4D printing [21–23]
have been well developed. Specifically, spray coating is a simple
and low-cost strategy suitable to various component dispersions,
but suffers from low printing resolution. Relatively, inkjet printing
with high precision is widely applied in many fields [11–13,24–
26]. Notwithstanding, the preparation of inkjet printing ink is very
difficult due to the demand of low concentration of binders with a
high viscosity that can prevent the blocking of nozzles of small-
⇑ Corresponding author.
E-mail address: wuzs@dicp.ac.cn (Z.-S. Wu).
1
These authors contributed equally to this work.
also realize high-resolution and large-area fabrication of MBs and
MSCs, but its wide application is substantially limited by complex
technique processes. 3D printing as another promising fabrication
technology can realize freeform prototyping and construction.
Especially, it can avoid the direct contact of squeeze nozzles to
ensure free-pressure and is able to fully print the electrode and
electrolyte for MBs, which can also infinitely increase the areal
loading of printed devices. However, the increasing areal (mass)
loading at the sacrifice of flexibility for wearable electronics. Pro-
gressing in the 3D printing, a more advanced 4D printing technol-
ogy has been emerging due to its nature of intelligence by 3D
printing on the smart materials, which can react to the stimulation
of temperature, pressure, magnetism, water and so on. Therefore,
4D printing will have a revolutionary impact on a broad range of
applications [27]. However, limited by the numbered smart mate-
rials, 4D printing technology has still large development room to
meet the needs of common applications. Considering the flexibility
and high areal loading of printed microscale energy storage
devices, screen printing can realize the flexibly printing on various
substrate and improve high areal loading by low-cost repeated
printing process compared with spray coating and 3D printing. In
addition, with the exploration of wide-range printable binders

https://doi.org/10.1016/j.jechem.2021.08.011
2095-4956/Ó 2021 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
Y. Zhang, Y. Zhu, S. Zheng et al.
and solvents, screen printing can also realize an increasing preci-
sion compared with the inkjet printing and transfer printing,
enabling it a promising technology for scalable fabrication of
microelectronics.
Screen printing, a simple operation by extruding the cus-
tomized ink on the rigid or flexible substrates, centers on its low-
cost, excellent operability, simple manufacture process and large-
scale production, which has been applied on diverse applications
[28]. The major challenge of large-scale applications for high-
throughput fabrication fields ranging from batteries, supercapaci-
tor and sensors is to prepare functional ink. Further, the eco-
sustainable screen-printing technology is mainly dependent on
‘‘green-ink” by tuning the suitable binders and solvents [29].
Therefore, the aqueous screen-printing ink is more suitable for
large-scale manufacturing of wearable microelectronics. So far,
the commonly used solvents for printed ink are the water and
organic solvents, while the binders are depended on the viscosity
and functionality. The viscosity of the ink is related to the binder
to ensure that the ink is firmly attached to the substrate without
clogging the mesh of the screen fabric. In addition, the functional-
ity of the binders is becoming more and more important for the
formation of the ink. For example, in the graphene-based ink, the
binders should contribute an electrostatic repulsion to avoid the
easy aggregation of graphene nanosheets. Hence, the comprehen-
sive consideration should be drawn for the excellent properties
of screen-printing ink with appropriate rheological properties to
apply alterable application requirements. Apart from the fabrica-
tion of the designed ink, screen printing allows a wide range of
printing materials (e.g., particles, one-dimensional (1D) carbon
nanotubes, two-dimensional (2D) materials) and optional sub-
strates (e.g., paper, poly(ethylene terephthalate) (PET), textiles,
Fig. 1. Schematic illustration of screen-printed ink and their printed microelectronics applications. Inset images: Solvents, Reprinted from Ref. [39] with permission of Royal
Society of Chemistry. Binders, Reprinted from Ref. [40] with permission of Wiley & Sons, Inc. Additives, micro-batteries, Reprinted from Ref. [41] with permission of Wiley &
Sons, Inc. Micro-supercapacitors, Reprinted from Ref. [7] with permission of Wiley & Sons, Inc. Micro-sensors, Reprinted from Ref. [42] with permission of Wiley & Sons, Inc.
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Journal of Energy Chemistry 63 (2021) 498–513
glass) [30–32]. Based on these appealing features, screen printing
is widely applied for the rapid and scalable fabrication of
microelectronics.
As the rapid development of printed electronics in recent years
[31,33–38], there are few reviews on screen printing to detailly
introduce the fundamental of blade coating and summarize the
preparation of ink components and key applications in different
printed microelectronics. Herein we review the recent progress
of ink formation, scalable applications, and challenging perspec-
tives of screen printing for emerging printed microelectronics.
Firstly, we systematically summarized the fundamental of screen
printing, the rheological property of the inks influenced by the sol-
vents and binders. Furthermore, we summarized the application of
customized screen-printing ink in different printed micro-devices,
such as MBs, MSCs, and micro-sensors (Fig. 1). Finally, the perspec-
tives and future challenges of screen printing for printed micro-
electronics are highlighted, with a focus on a mission of
flexibility, safety and intelligence.
2. Fundamental and ink formation of screen printing
Among all printed fabrication methods for microelectronics
devices, screen printing is known for its superiority of low cost,
customizable pattern, excellent compatibility with flexible sub-
strate and large-scale productions. However, the manufacturing
parameters such as the rheology, printed resolution and film thick-
ness, and ink composite including the fillers, binders and solvents
of screen printing are rarely summarized. In this section, we will
introduce the fundamental process and key components of screen
printing in details.
Y. Zhang, Y. Zhu, S. Zheng et al.
2.1. The fundamental of screen printing
The screen-printing process is mainly completed under the
coordination of the screen fabric, squeegee, mesh, and ink. In a typ-
ical screen printing process, the screen stencil is firstly firmly fixed
at the screen printing machine. Next, the ink is placed on one side
of the printed pattern on the screen, and squeezed in virtue of the
force of the squeegee onto the substrate. Finally, the desired pat-
tern as same as variable mesh was readily formed (Fig. 2). Although
screen printing is one of the most widely used printing techniques
and its process is simple, the quality of printed films (e.g., resolu-
tion, adhesion to substrate, thickness) are determined by multiple
factors. The patterning resolution is one of important properties of
screen-printed films, which mainly depends on the numbers and
materials (e.g., polyester fibers, stainless steel) of the meshes con-
sidering that the screen-printed patterns is the direct replication of
meshes. In addition, it is also determined by the ink rheology to
ensure high precision with fine edges through the mask without
dispensing out the pre-patterned area. Apart from the resolution,
the adhesion of printed films is influenced by surface tension and
wettability of printable inks to targeted substrates, which could
be adjusted by the used solvents and binders [30,33,34]. Besides,
the thickness of printed films, as another significant factor, is up
to the mesh number of screens, thickness of screen fabric and ink
composition. In fact, the screens are prepared by a standardized
production process, so there is no sufficient space to change the
properties of screens. On basis of this, the research efforts in
screen-printed film enhancement are mainly focused on ink mod-
ulation including active materials, solvents, binder and conductive
additives, which will be discussed in detail as follows.
2.2. Screen-printed inks
The ink for screen printing is typically composed of the fillers,
binders and solvents, which can be coordinated in a suitable pro-
portion to guarantee a proper viscosity that sometimes depends
on the type of substrates, e.g., metals, wood, fabric, glasses, ceram-
ics, polyethylene terephthalate, and paper [41,43]. One of the main
challenges of printed microelectronics is the development of func-
tional ink. However, the viscosity of screen-printing ink is mainly
determined by the type and proportion of selected binders, which
determines the ink rheological properties when printing at differ-
ent substrates. At present, the binders are mainly divided into
organic and aqueous binders. Taking into account of environmental
protection, the aqueous binders have received extensive attention.
Fig. 2. Process schematic of screen printing.
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Journal of Energy Chemistry 63 (2021) 498–513
Ink rheology is an important index to evaluate the performance
of ink, which can be largely determined by the content of ink fillers,
solvent ratio and binder types (Table 1). In addition, the physical
and chemical stability of the ink is also affected by the different
manufacturing methods and procedures, such as the temperature
and time of stirring or dispersion [33,38].
2.2.1. Composition of screen-printed inks
The solvents play a core role for the rheological property of ink.
So far, most screen printed inks select organic solvents (Table 1),
such as toluene [40], tetrahydrofuran [44,68], dimethylsulfoxide
(DMSO) [45], N-methyl pyrrolidone (NMP) [46–48], DMF [49],
propylene glycol [50], glycol [51], 2-propanol [52], and ethanol
[40,53], which are volatile, poisonous, and environmentally
unfriendly, preventing the wide application for wearable electron-
ics. Toluene was selected as the polystyrene-block-polyisoprene-
block-polystyrene (SIS) solvent due to its similar Hillenbrand solu-
bility parameters [40]. The NMP [46–48] has become an exten-
sively applied solvent for the preparation of ink due to its low
volatility, good thermal and chemical stability and excellent com-
patibility with most organic and inorganic compounds. For
instance, the NMP is combined with tetrahydrofuran as a solvent
to construct the silver and graphene ink [44,68]. However, with
the sustainable development and green initiatives, these organic
solvents are not the best choice for ink preparation due to its tox-
icity and non-environmental friendliness. Hence, it is very urgent
to find a ‘‘green solvent” that can not only achieve high solubility
and stability of fillers, but also meet the needs of health and envi-
ronment. Recently, great efforts have been devoted to explore
potential and multifunctional solvent substitutes, such as deion-
ized water [7,56–64] and bio-based solvents [54,55]. Accordingly,
dihydrolevoglucosenone (Cyrene) with non-toxic and friendly to
human health [39,48] was reported as a potential replacement
for organic solvent of NMP (Fig. 3a). Especially for the ultrahigh
concentration of graphene screen-printing ink, the Cyrene pro-
vided a better dispersion and a lower risk of structural damage
of graphene under continuously ultrasonic process compared to
NMP solvent (Fig. 3b) [39]. It also can be specially demonstrated
by the Raman spectroscopy results (Fig. 3c). Further, Costa et al.
developed a solvent of N,N’-dimethylpropyleneurea (DMPU) with
excellent chemical stability and superb dissolving ability to many
organic and inorganic compounds and even some polymers for
printing ink. The rheological properties of the ink were compared
with the ones with the conventional solvent NMP, indicating a
more pronounced shear-thinning behavior than the NMP ink
Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

(Fig. 3d) [67]. Additionally, the terpinol has the advantages of low
curing point (
40 ℃), high boiling point (217 ℃), natural composi-
tion, colorless and tunable viscosity, regarding as a green-health
solvent for graphene ink and Pb3O4 ink (Fig. 3e) [54,55].
Considering the unfriendly to health for low toxicity organic
solvents, deionized water [7,56–64] with the nature of high-level
safety has been considered a promising ink solvent in the future.
For instance, Yu et al. reported a MXene ink using deionized water
as the solvent for the fabrication of MXene based MSCs via screen
printing technology (Fig. 3f). The MXene ink exhibits a shear-
thinning behavior in which the viscosity decreases with increasing
shear rates, and the ink possesses high viscosity of >104 Pa s at a
shear rate of 0.05 s
1 (Fig. 3h). In addition, according to the curves
of storage modulus (G0 ) and loss modulus (G00 ) of the ink, as well as
the oscillatory frequency sweep results (Fig. 3i and j), it is indicated
that the MXene-N ink can flow continuously on various substrates
and be printed with the well-defined patterns (Fig. 3g) [7]. This
result provided a distinctive insight to harnessing such green-
health solvent of deionized water into the printable ink with supe-
rior rheological property.
Apart from the solvents, the binders play an important role in
the screen-printed inks. The appropriate binder can ensure that
the ink is fluently printed on different complex substrates. So far,
according to different application needs, organic-based and
water-based binders have been widely studied. Polymeric materi-
als, such as the SIS [40], polycarbonate (PC) [49,68], and thermo-
plastic polyurethane polymer (TPU) [44], Nafion [52],
polyvinylidene fluoride (PVDF) [46,47] and PTFE binder [53] have
been commonly used as the binders for screen printing technology
to realize functional properties during the adjustment of proper
adhesion of the ink. This section will be covered in detail in the
next section.
To further improve the electrical conductivity of the ink, con-
ductive additives, such as carbon black [47,56,63], acetylene black
[58], graphite [64] and carbon nanotubes [52,65,66], are commonly
used. Typically, for some non-metallic inks, graphene is widely
applied in the preparation of screen-printing ink due to its high
electrical conductivity and 2D laminated structure to produce a
planar conductive network to improve the electrical conductivity
of microelectronics [53]. Further, in order to form a highly conduc-
tive network, 1D carbon nanotubes combined with 2D graphene
served as a high conductive bridge to conduct a three-
dimensional conductive network, which can together enhance
the conductivity of the printed microelectronics [65,66]. For some
metallic inks, graphene is usually selected as a conductive additive
to connect metal particles and achieve better printing effects [57].
In addition, active materials are mainly divided into battery mate-
rials, sensing materials and conductive carbon materials according
to different applications.
2.2.2. Organic screen-printed inks
For organic screen-printed inks, the choice of the binder is cru-
cial. Due to the special molecular chain structure of organic binder,
much attention has been paid in some special fields. In particular,
owing to the unique block polymeric structure of short polystyrene
terminal ends and long polyisoprene chain which can lead to the
cross-linking under high temperature, the SIS has superior elastic-
ity and mechanical strength, as well as excellent flexibility at low
temperature of
65 °C. Benefiting from the unrivaled properties
of SIS, a stretchable Zn-Ag2O battery exhibited attractive hypere-
lastic properties (1300% elongation). Based on the superiority of
SIS, the stretchable batteries still maintained the prominent elec-
trochemical and mechanical properties (Fig. 4a and b) [40].
On the other hand, the organic binders have special functions,
especially used in the ink of lamellar structural materials. For

Table 1
Summary of the typical binders, conductive additives and solvents of various screen-printed inks.

Ink Binders Conductive additives Solvents Refs.

Zn/Ag2O ink SIS Super-P 80% Toluene + 20% [40]
ethanol
Silver and graphene ink TPU Silver flakes and graphene DMF + THF [44]
nanoplatelets
RuO2 ink Poly(4-styrenesulfonic acid) rGO DMSO + DI water [45]
Conductive carbon ink PVDF Carbon NMP [46]
LFP ink PVDF Carbon black NMP [47]
Cyrene-based graphene ink/ NMP-based CAB - Cyrene/ NMP [48]
graphene ink
h-BN ink PC - DMF [49]
AgNWs ink (hydroxypropyl)methyl cellulose AgNWs DI water + propylene [50]
glycol
Graphene ink N-vinyl-2-pyrrolidone and vinyl - Dipropylene glycol [51]
acetate
Carbon ink Nafion Carbon 2-propanol [52]
NGP/PANI ink PTFE Nanotube graphene platelets Ethanol [53]
mGO ink PVP mGO Terpineol [54]
Pb3O4 ink Ethyl cellulose - Terpineol [55]
Ag@PPy@MnO2 and AC ink Waterborne resin Carbon black DI water [56]
N-Doped MXene ink LA132 binder Super P DI water [7]
AgNWs ink - AgNWs-GO DI water [57]
FeOOH/MnO2 ink Polyacrylic latex Acetylene black DI water [58]
AgNWs ink (hydroxypropyl)methylcellulose AgNWs DI water [59]
Activated Carbon ink Chitosan Activated carbon DI water [60]
Graphene ink CMC-Na - DI water [61]
PEI-rGO ink Waterborne polyurethane - DI water [62]
LFP/ Graphite ink CMC/ Cellulose nanofibers Carbon black DI water [63]
Graphite ink CMC + MFC Graphite particles DI water [64]
MWCNT/PEDOT:PSS ink PEDOT:PSS MWCNT Milli-Q ultrapure water [65,66]

Note: polystyrene-block-polyisoprene-block-polystyrene (SIS), thermoplastic polyurethane polymer (TPU), polyvinylidene fluoride (PVDF), cellulose acetate butyrate (CAB),
polycarbonate (PC), polytetrafluoroethylene (PTFE), carboxymethylcellulose sodium salt (CMC-Na), carboxymethyl cellulose (CMC), microfibrillated cellulose (MFC), mul-
tiwall carbon nanotube (MWCNT), Ag nanowires (AgNWs), dimethylformamide (DMF), tetrahydrofuran (THF), dimethylsulfoxide (DMSO), deionized (DI), N-methyl-
2pyrrolidone (NMP), poly(3,4-ethylene dioxythiophene):poly (styrene-sulfonate) (PEDOT:PSS), polyaniline (PANI), nano graphene platelets (NGP).

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Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

Fig. 3. The composition of screen printed inks. (a) 3D molecular models of CyreneTM. (b) The comparative concentration of graphene dispersed in Cyrene and NMP. (c)
Comparison of graphene quality when sonicating in the solvents of NMP and CyreneTM with varying sonication times. (a-c) Reprinted from Ref. [39] with permission of Royal
Society of Chemistry. (d) Variation of viscosity with shear rate of the anode ink prepared with NMP (solid symbols) and DMPU (open symbols). (e) Cross-section SEM image of
2.25/DMPU/SP. (d-e) Reprinted from Ref. [67] with permission of Elsevier. (f) The screen printing fabrication process for MXene MSCs. (g) Photographs of MSCs at bent and flat
states by printing MXene on various substrates. (h) Viscosity of MXene ink as a function of shear rate. The storage modulus (G0 ) and loss modulus (G00 ) of MXene ink as
functions of (i) shear stress and (j) angle frequency. (f-j) Reprinted from Ref. [7] with permission of Wiley & Sons, Inc.

example, PC as an organic binder characteristic of functional poly-
mer chains has been utilized in preparing hexagonal boron nitride
(h-BN) ink. This functional chain of polymer macromolecules
adsorbed on the lamellar materials by means of steric hindrance
effect to enable the lamellar materials dispersing well. Therefore,
the PC polymer prevented further aggregation of the lamellar h-
BN materials during centrifuging at a higher viscosity, resulting
in a shear-thinning behavior for h-BN ink (Fig. 4c-f) [49]. Also,
TPU with high optical transparency, excellent mechanical strength,
and good solubility in various organic solvents was selected as the
binders to produce the viscoelastic ink for wearable electronics
[44]. In addition, the PVDF with the merits of high impact tough-
ness, corrosion resistance and adjustable viscoelasticity was
widely applied to the manufacture of conductive carbon ink
printed as a carbon-based current collector [46] or an electrode
ink [47]. Nafion, depending on excellent thermal and chemical sta-
bility, as well as mechanical strength, has been applied for a
screen-printed cathode for nonaqueous Li-O2 batteries. It is noted
that Nafion is firstly lithiated by using lithium hydroxide aqueous
solution to fabricate the cathode ink. The lithiated Nafion ionomer
owns a stronger crosslinking due to the interaction between the Li
ion and hydrogen in the sulfonate group of Nafion [52].
As we known, a binder is usually added to the ink, which has a
certain adhesion to ensure that the ink can be firmly printed on the
substrate. For example, it is very unfavorable to the preparation of
graphene ink, owing to the restacking and aggregation of graphene
nanosheets. To solve this problem, Hu et al. ingeniously selected
cellulose acetate butyrate (CAB) as a binder into the graphene
ink, which can stabilize the ink by the electrostatic repulsion
between graphene and CAB molecules (Fig. 4g-i) [48]. In addition,
considering the graphene deposition and green-sustainable, Wang
et al. chose a bio-based polymer, carboxymethylcellulose sodium

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Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

Fig. 4. The properties of organic screen printed inks. (a) A screen-printed Zn-Ag2O battery selected SIS as a binder. (b) Pictures of the Zn-Ag2O battery printed on a stretchable
textile while being different stretched states. (a and b) Reprinted from Ref. [40] with permission of Wiley & Sons, Inc. (c) Viscosity of the h-BN ink as a function of shear rate
and the photographs of the ink in the inset. (d) Photographs of the printed h-BN ink on the PET substrate and (e and f) the different magnified SEM images of the printed
patterns. (c-f) Reprinted from Ref. [49] with permission of American Chemical Society. (g) Preparation process of exfoliated graphene ink using Cyrene. (h and i) SEM images
of (h) uncompressed and (i) compressed screen-printed graphene flakes. (g-i) Reprinted from Ref. [48] with permission of Nature publishing group.

salt (CMC) to prevent the aggregation of graphene nanosheets [61].
In addition, another bio-based polymer, chitosan has a variety of
physical and chemical functions, such as biodegradability, biocom-
patibility, and non-toxicity, which enables it a potential binder
candidate for printed electronics. By applying chitosan as binder,
activated carbon (AC) ink was synthesized to fabricate screen-
printed aqueous supercapacitors with high stability and operatable
voltage [60].
2.2.3. Aqueous screen-printed inks
Taking into account of the green sustainable development,
human health, and environmentally friendly in the screen-
printing post-processing process, the aqueous binders, possessing
the merits of low cost and environmentally friendliness, are con-
sidered as the most ideal candidate. Usually, it is relatively com-
mon that adding binders is to enhance the adhesion in the
preparation of inks. However, the effect of binders on electrical
conductivity should be emphasized. Practically, the addition of
binders is usually not conducive to the improvement of ink con-
ductivity, or even negatively related to electrical conductivity
[48]. To overcome this problem, Nørgaard et al. presented a reliable
approach for printing ink by adding mildly oxidized graphite
(mGO) into polymeric binder of polyvinylpyrrolidone (PVP) that
have not destroyed the electrical conductivity of ink. Meanwhile,
the sheet-resistances (RS) can be enhanced by two orders of mag-
nitude under compression (Fig. 5a) [54]. Hence, this aqueous bin-
der has a certain contribution to the improvement of electronic
conductivity.
As a water-dispersible binder, the viscosity can be easily
adjusted by changing the proportion of water, the monomer struc-
ture and molecular weight of aqueous binders [45]. An aqueous
binder of PSS can achieve a high viscosity by adjusting the mono-
mer concentration and molecular weight of PSS. In addition, PSS
can also realize the good dispersion of various materials and uni-
form anchoring through electrostatic repulsion interactions by vir-
tue of its sufficient sulfonate groups (-SO3-). Accordingly, PSS was
selected as a polymeric binder to construct a PEDOT:PSS/graphene
ink to improve the charge-transport performance and viscosity.
Notably, this binder allows stable dispersion of nanoparticles and
graphene in an aqueous PEDOT:PSS ink through electrostatic stabi-
lization. Therefore, PSS is a promising polymeric binder for opti-
mizing the viscosity of PEDOT:PSS solution to realize the
homogeneous printing on various flexible substrates (Fig. 5b) [45].
Apart from the tunable viscosity, the binders should also be ver-
satile, enabling the reduction of graphene and strong bonding of
graphene to the binders. However, graphene ink requires harsh
post-treatments owing to the low electrical conductivity of GO,
which restricts GO as a substrate for widely application. Recently,
Gao et al. reported that butane tetracarboxylic acid (BTCA) and
sodium hypophosphite (SHP) were applied to reduce GO and
establish a tenacious chemical bond between reduced GO (rGO)
and viscose fibers after the screen-printing process (Fig. 5c). Inter-
estingly, the depth of fabric penetration and GO states were also
tuned through the control of the concentration of GO ink, resulting
in higher viscosity of GO ink with low penetration depth (Fig. 5d).
Further, these nonwoven fabrics printed by rGO ink exhibited high
electrical conductivity when applying to physical sensors [69]. This

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Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

Fig. 5. The properties of aqueous screen-printed inks. (a) Sheet resistances of films under different compressed states. (a) Reprinted from Ref. [54] with permission of Wiley &
Sons, Inc. (b) Fabricating process of RuO2/PEDOT:PSS/graphene screen-printed electrode. (b) Reprinted from Ref. [45] with permission of American Chemical Society. (c) The
aqueous GO ink and the fabrication process of nonwoven fabric-based sensors. (d) Schematic structures and corresponding SEM images of pure fiber, GPC-F with different
concentration of GO. (c and d) Reprinted from Ref. [69] with permission of American Chemical Society. (e) Molecular structures of (hydroxypropyl)methyl cellulose and Zonyl
FC-300. (f) Variation of viscosity for Ag nanowire (AgNW) ink with shear rate. (g) Viscosity as a function of time for the ink. (e-g) Reprinted from Ref. [50] with permission of
Wiley & Sons, Inc. (h) Schematic diagram of the fabricating process of WPU/PEI-rGO composites and procedure of screen printing. (h) Reprinted from Ref. [62] with
permission of Royal Society of Chemistry.

approach not only achieved GO reduction through a simple print-
ing process by adding special reagents, but also strongly adhered
the ink to the fabric, which was worthy of further promotion for
printed microelectronics.
Necessarily, the binder’s transparency and high viscoelasticity
are of great importance for printed electronics. For instance, Pei
and co-workers reported highly conductive Ag nanowires (AgNWs)
ink composed of hydroxypropyl methylcellulose, antifoaming
agent and fluorosurfactant (Fig. 5e). Further, the fluorosurfactant
served as a regulator of surface tension of ink to promote the adhe-
sive ability of ink to the printing substrates. Also, hydroxypropyl
methylcellulose as a viscoelastic polymer with high transparency
and stable performance can provide thixotropic behavior for the
ink. Besides, distilled water in this work was selected as a ‘‘green”
solvent due to its environmental friendliness and low cost. All the
features of this water-based AgNWs ink produced a shear-thinning
thixotropic behavior for three ink distinguished by the AgNWs
solid contents (Fig. 5f and g) [50]. In addition, due to the high
transparency and stable performance of hydroxypropyl methylcel-
lulose, it is very popular in AgNWs ink. Recently, a screen-printable
AgNWs ink with high conductivity (up to 8.32  103 S cm
1) by
selecting hydroxypropyl methylcellulose as binder was reported
by Lai et al. [59]. It is noted that the AgNWs ink possessed suitable
rheological behaviors and showed high resolution (100 mm) and
favorable optical transmittance (80%) when screen printed on
flexible substrate.
To adapt to the eco-environmental requirements, the ink of
screen printing plays a crucial role in the manufacturing of printed
products. Recently, waterborne polyurethane reported by Zhang
et al. [62] is a safe, reliable and environment-friendly polymer
material with excellent mechanical properties and compatibility.
What’s more, the viscosity of waterborne polyurethane is generally
adjusted by water-soluble thickeners and water. Due to its health
and environmentally friendly properties, the ink can be well used

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in many fields. Specifically, Zhang et al. proposed a polyethylenei-
mine graphene-modified surface-tailored graphene (PEI-rGO) ink
utilizing waterborne polyurethane to achieve scalable manufactur-
ing of screen printing (Fig. 5h). Apart from the waterborne polyur-
ethane, waterborne resin [56], LA132 binder [7] and polyacrylic
latex [58] have been got attention due to the superiority of easily
soluble in water, low toxicity, and environmentally friendliness.
3. Screen-printed microelectronics
3.1. Screen-printed micro-batteries
The sustainable development of flexible energy storage devices
requires a high-safe energy supply and low-cost fabrication tech-
nology. The commonly used manufacturing methods, such as 3D
printing and photolithography, have provoked tremendous devel-
opment of MBs in the past few years, but their commercial appli-
cations were still limited by high cost, rigorous technical and
equipment requirement, as well as complicated manufacturing
process. Screen printing is cost-effective, processable flexibility
and easy operation. Therefore, it has been applied for the fabrica-
tion of various MBs (Table 2), such as Zn-Ag2O batteries [40],
lithium-ion micro-batteries (LIMBs) [47,63,64,67,70–74,78], Zn/
Ag battery [46,75], and Zn/MnO2 battery [43]. Furthermore, screen
printing technology has been extended to produce printable elec-
trolyte membranes and all-solid-state batteries. So far, various pos-
itive electrode materials have been exploited for screen printing
LIMBs, such as LiCoO2 [71–74], LiMn2O4 [78], lithium metal phos-
phates (LiFePO4, LiMnPO4 and LiCoPO4) [47,63,67], and vanadium
oxides [79]. The active materials with different size and morphol-
ogy make an impact on the thickness of screen-printed MBs. The
larger active material particles will increase the thickness of MBs
and need a larger mesh of printing screen, which directly affected
the long-range dynamics of Li ion migration, resulting in low speci-
fic capacity of the cell. Also, the porosity of the active material ink
will affect the performance of printed MBs by influencing the adhe-
sion and exfoliation of active materials.
Recently, the printable ink has been conducted for aqueous Zn//
MnO2 MBs and LIMBs by screen printing. An aqueous printable
Zn//MnO2 MBs with characteristic of high-safety, prominent flexi-
bility, and excellent performance has been reported by Wang et al.
[43]. The printable aqueous Zn//MnO2 MBs with an interdigital
microelectrode design delivered a notable volumetric capacity of
19.3 mAh cm
3 at 7.5 mA cm
3 (Fig. 6a and b). Moreover,
MXene-based LIMBs have been fabricated by printing aqueous-
based ink, which are combined MXene and electrode materials of
lithium titanium oxide (LTO) as anode and lithium iron phosphate
(LFP) as cathode in the interdigital planar geometry to realize an
interbedded structure interlining lamellar MXene and electrode
particles (Fig. 6c and d). The printable LIMBs offered a high areal
energy density of 88 lAh cm
2 at a current density of 20 lA cm
2
(Fig. 6e) [41]. Based on the excellent electrochemical performance
of these printable MBs, screen printing technology will open a new
avenue to facilitate the environmentally friendly and high-safe
MBs.
Apart from the Zn//MnO2 MBs and LIMBs, the flexible nickel-
metal hydride (NiMH) battery has been also fabricated by screen
printing [77]. To improve electrochemical performance of the flex-
ible NiMH battery, the fabrication of a flexible and poriferous
nickel matrix is the prerequisite. In order to obtain the porous
structure of nickel, flexible porous nickel matrix has been firstly
printed on the steel sheets using an insulating ink before nickel
electrodepositing on this insulating template (Fig. 6f). Profiting
from the novel manufacturing method of porous structure by
screen printing, flexible NiMH batteries displayed excellent energy
density of 151.8 Wh kg
1, demonstrating the promise of screen
printing in application of NiMH batteries (Fig. 6g).
Besides, two stretchable Zn-Ag2O battery with a ‘‘NANO” design
has been manufactured using screen printing technology by a cus-
tomize Zn/Ag2O ink selected SIS as a binder (Fig. 7a). It is observed
that the strain mapping showing a significant difference when the
rectangular carbon electrodes (1:3 ratio) is stretched from 0% to
100% stretching (Fig. 7b, c). Obviously, the pristine battery shows
a discharge capacity of 3.78 mA h cm
2, and the stretching battery
slightly increases by 3.94 mA h cm
2 whereas the average voltage

Table 2
Summary of electrochemical performance of various micro-batteries fabricated by screen printing technology.

Battery types Cathode Anode Current collectors Separator and electrolyte Capacities Refs.
Li ion LiFePO4 Li Al foil Whatman glass microfiber/1M LiPF6 in EC-DEC 48.2 mAh g
1 (5C, cathode) [47]
(1:1, v/v)
Li ion C-LiFePO4 Graphite Al foil (cathode), Whatman glass microfiber/1M LiPF6 in EC-DEC 52 mAh g
1 (2C, cathode), [67]
Cu foil (anode) (1:1, v/v) and 349 mAh g
1 (C/5,
anode) after 50 cycles
Li ion Ag-doped Zr- Li or Fe/Si - 1 M LiPF6 in EC/DEC (1:1, v/v) 250 lAh cm
2 [70]
LiCoO2 (100 lA cm
2)
Li ion LiCoO2 Li Pt PP separator/1 M LiPF6 in EC/DEC (1:1, v/v) 179 lAh cm
2 (80 lA cm
2) [71]
Li ion LiCoO2 Li Pt PP separator/1 M LiPF6 in EC/DEC (1:1, v/ 125 lAh cm
2 (80 lA cm
2) [72]
v) + LiPON solid electrolyte
Li ion LiCoO2 Li - Nb-Li7La3Zr2O12 + Li3BO3 solid electrolyte 85 mAh g
1 (10 mA cm
2) [73]
Li ion LiCoO2 Graphite C/Al + Cu Gel polymer electrolyte 2.5 mAh cm
2 [74]
Li ion LiFePO4 Graphite Cu 1 M LiPF6 in EC-DMC (1:1, v/v) 80 mAh g
1 (0.1C) [63]
Li ion Graphite Li - 1 M LiPF6 in EC-PC-DMC (1:1:3, v/v/v) 100 mAh g
1 (0.1C) [64]
Zn/air PEDOT Zn/carbon/ - 12 M LiCl + 0.1 M LiOH solution 1.4 mAh cm
2 [68]
polymer
Ag/Zn Ag Zn Carbon 3% PAA containing 6 M KOH + 1 M LiOH (Ag)/ 1.3–2.1 mAh cm
2 [75]
10% PAA-K containing 6 M KOH + 1 M LiOH
(Zn)
Ag/Zn Ag Zn Carbon Gel-based electrolyte 1.2 mAh cm
2 (4 mA cm
2) [46]
Zn/ Ag2O Ag2O Zn Carbon Gel-based electrolyte 2.5 mAh cm
2 (3 mA cm
2) [40]
Zn/MnO2 MnO2 Zn Graphene 2 M ZnSO4 + 0.5 M MnSO4 19.3 mAh cm
3 [43]
(7.5 mA cm
3)
Polymer battery PEDOT:PSS PEDOT:PSS/PEI - PSSNa 5.5 mAh g
1 [76]

Note: poly acrylic acid (PAA), poly(3,4-ethylenedioxythiophene) (PEDOT), polyethyleneimine (PEI), poly (styrene sulfonate sodium) (PSSNa).

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Fig. 6. Screen printing fabrication of MBs. (a) Schematic of fabrication for printable Zn//MnO2 planar MBs by screen-printing. (b) GCD profiles of printable Zn//MnO2 MBs. (a
and b) Reprinted from Ref. [43] with permission of the Oxford University Press. (c) Schematic fabrication of MX-LIMBs using MXene-based LTO and LFP inks. (d) Structure of
the printed microelectrodes for MXene-based batteries. (e) Electrochemical performance of printed MXene-based batteries. (c-e) Reprinted from Ref. [41] with permission of
Wiley & Sons, Inc. (f) The screen printing process to fabricate the template and the porous nickel films. (g) Charge and discharge curves at different current rates. (f and g)
Reprinted from Ref. [77] with permission of Wiley & Sons, Inc.

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Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

Fig. 7. Screen printing fabrication of Zn-Ag2O and thin-film batteries. (a) A Zn-Ag2O battery fabricated by screen printing technology. (b and c) 2D mapping of the stretched
electrodes. (d) GCD profiles of the stretchable battery. (e) The discharge capacity under pristine and stretching. (a-e) Reprinted from Ref. [40] with permission of Wiley & Sons,
Inc. (f) Fabrication process, (g) initial GCD curves, and (h) flexibility testing for the printable thin-film Li-ion battery. (f-h) Reprinted from Ref. [74] with permission of Elsevier.

decreases slightly after stretching. The increased capacity is ization (Fig. 7d). Remarkably, the prominent mechanical properties
ascribed to the enlarged active surface area after stretching, while of the SIS binder enable the Zn-Ag2O battery an outstanding flexi-
the decreased voltage is caused by ascribed to the increased polar- bility, which can resist a severe tension and present a high capacity

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Y. Zhang, Y. Zhu, S. Zheng et al.
of 2.5 mAh cm
2 (Fig. 7e) [40]. Screen printing technology can print
on flexible substrates to realize excellent flexibility and electro-
chemical properties, which is respected a promising candidate
for flexible microelectronics.
The screen printing technology has been also applied for thin-
film Li-ion battery. A pouch-type flexible thin-film Li-ion battery
is designed by sequentially screen-printing the current collector,
cathode, anode and gel polymer electrolyte (Fig. 7f). This interest-
ing thin-film Li-ion battery using dry-wet processes exhibits an
energy density of 332.8 Wh L
1 based on metallic of Al and Cu
as the current collector (Fig. 7g) and high capacity retention of
84% after 50th cycles. The flexibility is also evaluated by consider-
ing the fluctuation of open-circuit voltage, resulting in a stable
fluctuation under the state of folding, bending and stretching
(Fig. 7h). The high capacity and flexibility enable the feasible and
predominant screen printing technology a promising strategy for
promoting the development of thin-film lithium-ion battery [74].
Besides, screen printing is a low-cost, easy-to-operate manufactur-
ing technology for MBs with thick film electrode. In terms of these
characters, Lee et al. reported Zr-doped LiCoO2 thick films up to
20 lm by a screen-printing process [70]. In order to attain high
energy density, both of the thick and smooth surface for screen-
printed LiCoO2 films should be considered synchronously. The
rougher the surface, the greater the risk of an electrochemical short
circuit. However, the annealing process may cause an uncontrolled
structure of the printed electrode hole and increase the surface
roughness of the films. Based on the drawbacks, Park and cowork-
ers propose a strategy to manufacture the LiCoO2 thick film with-
out a post-annealing process. The LiCoO2 powder is coated with a
carbon layer by pyrolysis of the mixture of resorcinol and carbon
black, which can reduce the surface roughness of the printed film
and then obtain excellent performance with high discharge capac-
ity of 179 lAh cm
2 [71]. Also, an all-solid-state Li ion battery with
greater energy density can be achieved by a screen-printing pro-
cess. This all-solid-state lithium ion battery selected Nb-doped Li7-
La3Zr2O12 and Li3BO3 as a solid-state electrolyte by annealing,
which present better excellent performance than the traditional
liquid electrolyte. Traditional solid-state batteries have the draw-
back of large contact interface impedance between electrode and
solid electrolyte. However, the tighter bonding between solid-
state electrolyte and cathode can be efficiently realized by screen
printing combined with the later calcination process, thereby
reducing the surface impedance [73].
3.2. Screen-printed micro-supercapacitors
Due to the merits of fast charge and discharge capability, high
output power, long cycle life, easy production and integration,
MSCs have great potential as an on-chip microscale energy storage
unit. Furthermore, MSCs can be used as a supplement to battery
and energy collection system and a microscale power supply for
next-generation flexible on-chip electronic products [82–85]. High
performance-price ratio and high-throughput processing method
for large-scale production of electrode materials are crucial for
the wide application of MSCs. To this purpose, screen printing
has been extensively exploited in the production of planar MSCs
because of its inherent simplicity, good repeatability and high
compatibility with various functional ink and substrates [86–88].
Compared with the traditional sandwich structure, the interdigi-
tated planar MSCs provides several orders of magnitude higher
power density than batteries, so it is easy to be integrated into
miniaturized electronics for nano-/micro-level power source.
In order to realize the printable potential of supercapacitors on
an industrial scale, a cheap thin-film electrode production process
is highly needed. In general, screen printing is one of the most
extensive and significant industrial printing technologies for
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Journal of Energy Chemistry 63 (2021) 498–513
thin-film manufacturing. Most interestingly, the MSCs produced
by screen printing can be designed to display the required aes-
thetic characteristics [8,80,81,89], for example, parallel strip, inter-
digital, circular interdigital, and concentric circle shapes (Fig. 8a)
[80]. By designing a variety of line gap and shape patterns, hun-
dreds or thousands of high-resolution MSCs with conductive tracks
and letters can be printed quickly in a matter of seconds (Fig. 8i)
[90]. As a feasible manufacturing process, the development of high
quality and high conductive material ink is very important for
screen printing MSCs. A promising conductive ink should have
good printing performance, long-time stability, low cost and com-
patibility with diverse substrates, flexibility and tensile strain
resistance. To prevent the ink penetration and remain structural
integrity, screen-printed inks should possess high viscosity and
elasticity to assure its thixotropy and solid-like behavior. Typically,
graphene has high intrinsic conductivity, good mechanical prop-
erty, and expandable production capacity, making it a promising
conductive and electrode material for the formation of ink
[53,80,91]. For example, using highly-conducting graphene ink,
Wu et al. [80] directly screen printed customized and integrated
MSCs with designable shapes and size on any substrates, which
efficiently improved the working voltage and capacitance of MSCs
through series or parallel connection. Notably, an energy storage
pack with the serially connected 130 MSCs was capable of out-
putting a record voltage over 100 V (Fig. 8b). The screen-printed
graphene based MSCs can offer a high areal capacitance
(1.324 mF cm
2) and large volumetric capacitance

3
(0.490 F cm ), and remain stable electrochemical performance
after hundreds of cycles (Fig. 8f and g) [81]. Besides, the screen-
printed graphene patterns also serve as the current collector for
MSCs [92]. Further, screen-printing is developed for the construc-
tion of asymmetric MSCs based on ultrathin MnO2 nanosheets as
positive electrode and graphene as negative electrode, achieving
excellent flexibility and electrochemical performance, for example,
a high energy density (97.2 Wh kg
1) with capacitance loss less
than 3% after 10,000 cycles [89]. Additionally, graphene has been
used as the conductive network to carry active polymer materials
and formulate mixture ink, showing the industrial applicability
of screen printing technology in the manufacture of MSC elec-
trodes [53]. The voltage of single-cell VN//MnO2 asymmetric MSCs
comprising of VN and MnO2 interdigitated electrodes through a
sequential screen-printing method achieved a high voltage of
2.2 V, comparable to the most reported in-plane MSCs and asym-
metric MSCs [93]. Further, the MSCs via connection of two cells
in series can expand the output voltage to 4.4 V, twice of single
device. At the same time, by using parallel mode of two cells, the
capacitance can be doubled easily, which provides an advanced
modulation mode for device integration.
The main challenge of screen printing is to prepare printable ink
with suitable viscosity and rheological properties. In the most
cases, it is highly necessary to use inactive additives to prepare
electrode materials for printable ink, which will adversely impact
on the functional properties of MSCs [8,94]. More recently, Liang
et al. [57,95] developed the thixotropic ternary nano composite-
based printable ink containing 0D nanoparticles, 1D nanowires,
and 2D nanosheets, which enables them to make a viscous and col-
loidal ink without additional inactive additive. Besides, the screen-
printed MSCs from MXene composite ink without any inactive
additives exhibit high volumetric capacitances (864.2 F cm
3), out-
standing rate capability (304.0 F cm
3), excellent power density
(48.5 W cm
3) and energy density (13.5 mWh cm
3), and ultralong
cycle life (90% retention after 10,000 cycles) [95]. Interestingly,
Zhang et al. [8] reported an extensible screen-printing additive-
free 2D Ti3C2Tx MXene aqueous ink with appropriate rheological
properties (Fig. 8h). The MSCs based on MXene sediment ink pre-
sent excellent areal capacitance of 158 mF cm
2 and energy den-
Y. Zhang, Y. Zhu, S. Zheng et al. Journal of Energy Chemistry 63 (2021) 498–513

Fig. 8. Screen printing fabrication of planar MSCs. (a) Various screen-printed patterns of SPG-IMSCs on PET substrates. (b) The function between the output voltage of MSCs
and number of series units. (c) Photographs of SPG-IMSCs with twisted state, and the corresponding (d) tandem and (e) serial CV curves. (a-e) Reprinted from Ref. [80] with
permission of Royal Society of Chemistry. (f) Schematic diagram of MSCs accommodation into microfleece garment. (g) Electrochemical properties of MSCs after washing
cycle. (f and g) Reprinted from Ref. [81] with permission of Wiley & Sons, Inc. (h) Process diagram for screen-printed MXene-based MSCs and the optical image of (i) and
powering an LED light of (j), and the CV curves in (k) tandem and (l) serial shapes. (h-l) Reprinted from Ref. [8] with permission of Wiley & Sons, Inc.

sity of 1.64 mWh cm
2. These MSCs could be facilely connected in
series or parallel to boost the output voltage and capacitance
(Fig. 8c-e, i-l), and to construct integrated MSCs to meet specific
energy/power needs (Fig. 8j).
In the process of screen printing, the influence of the self-
stacking problem of 2D material ink on the performance of MSCs
is also considered. To address the self-stacking, Yang et al. [96]
developed a 3D boron carbon nitride (BCN) microsphere ink as
electrodes of MSCs. The areal capacitance of a single MSC reached
41.6 mF cm
2. The MSC also exhibited a remarkable mechanical
flexibility without obvious capacitance decay even upon bending
to 180°. Recently, the manganese hexacyanoferrate(MnHCF)-
MnOx-based ink, in which MnOx with hydrangea-like structure
grown on MnHCF nanocubes, was formulated to produce the flex-
ible MSCs [97]. Besides, different MSCs have been designed and
fabricated by screen printing diverse functional inks such as 3D-
network graphene/CoS2/Ni3S4(G/CoS2/Ni3S4) ink [98], amorphous
FeOOH/MnO2 ink [58], and nanoporous SnO2/CNT ink [99]. Due
to the rapid development of screen-printed inks and the advan-
tages of screen-printing technology, screen-printed MSCs are
anticipated as miniaturized energy-storage device, which can serve
as a micro-power source for self-powered, wearable and foldable
microelectronics.
3.3. Screen-printed micro-sensors
Apart from MBs and MSCs, screen printing technique could also
be used to construct flexible multi-functional micro-sensors [103–
106], including food inspection [107,108], environmental monitor-
ing [109,110], composition detection [111–113], clinical diagnosis
and monitoring [114–116]. Screen printed electrode stands out in
the sensor due to its small size, high integration and sensitivity.
Therefore, there is a growing demand for sensors to monitor a vari-
ety of environmental, physicochemical and biological parameters,
which needs the rapid progress of fabricating novel sensors with
advanced functions. Presently, screen printing technology is one
of the most extensively investigated procedures in the production
line of printed sensor. The screen-printed electrode of the sensor
has become an excellent substitute, overcoming the limitations
of traditional electrodes and meeting the demand for highly
repeatable and reproducible and sensitive detection methods, as
well as low production cost, flexible design, and small size. There
are many kinds of sensors made by the screen printing process,
and their inks are also diverse, typically, carbon materials
[107,113,117], metal nanomaterials [118,119], oxides [120,121],
and polymers [100,122]. Interestingly, adding nanomaterials or
enzymes among other compounds into the ink can extend the

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functions or enhancing properties of the sensors. In particular, the
integration of biomaterial-based responsive ink through screen
printing opens up a promising way for large-scale production of
responsive distributed sensing interfaces (Fig. 9a and b) [100].
Responsive ink formulations for bioactive biomaterials consist of
thickener, plasticizer, silk fibroin, and molecules such as pH indica-
tors or enzymes (among others). The sensors of bioactive inks
could reveal quantify chemicals (such as sweat and other body flu-
ids) released by the body or its surroundings by changing color.
The ink can be screen-printed in the fashion of high resolution
and complex patterns on textiles such as clothes, shoes and even
masks to provide detailed maps of the body’s exposure and rapid
response to chemicals. However, the air permeability, washability
and large-scale production still remain challenges for most elec-
tronic textiles. To this end, Li et al. [101] fabricated a washable
E-textile with high electrical conductivity and high air permeabil-
ity, and showed its appliance as a self-powered triboelectric ges-
ture textile (Fig. 9c-e). The E-textile can be mass-produced on
ordinary fabrics and display outstanding stability after washing.
In the future, this kind of electronic fabric is expected to play a
more and more important role in wearable electronics, smart
home, sensors, Internet of things, medical and other fields.
Soft pressure sensor is one of the indispensable devices in the
application of robot technology and printed microelectronics. The
conductive screen-printed ink by combining PEDOT:PSS with bis(
trifluoromethane)sulfonimide lithium salt was used to construct
the capacitive sensor with pressure sensitive (Fig. 9f-h) [102].
Owing to high conductivity, PEDOT:PSS is exploited and added into
ionic additive bis(trifluoromethane) sulfonimide lithium salt to
ameliorate the stretchability. Besides of the ink, the substrates
for screen printing are also evolving. To entirely substitute the tra-
ditional stiff or unreliable printed circuit substrates, Jerald Yoo

Fig. 9. Screen printing fabrication of micro-sensors. (a) Schematic diagram of screen printing with biomaterial-based ink and different types of substrates. (b) Photograph of
the pH-sensing screen-printed T-shirt. (a and b) Reprinted from Ref. [100] with permission of Wiley & Sons, Inc. (c) Schematic diagram of washable electronic textile (WET) by
screen printing. (d) Schematic illustration of WET producing a signal. (e) Isc and Voc of the WET as a function of different frequencies. (c-e) Reprinted from Ref. [101] with
permission of American Chemical Society. (f) Fabrication process of soft capacitive pressure sensor array. (g) Schematic illustration and (h) photograph of the soft capacitive
pressure sensor. (f-h) Reprinted from Ref. [102] with permission of Wiley & Sons, Inc.

510
Y. Zhang, Y. Zhu, S. Zheng et al.
et al. [123] recently proposed the bio-degradable medical hydro-
colloid dressing (3 M Tegaderm) as the passive and interconnected
platform for screen-printing wearable sensors. Screen-printed sen-
sors were also exploited to develop robot sensors that mimic
human perception. The electrochemical device with taste-sensing
finger was printed on a robotic glove simulating soft skin, which
could realize real-time data transmission by integrating with the
wireless electronic board [107]. The ‘‘spicy” and ‘‘sour” fingers rely
on carbon electrodes, and various catalytic nanomaterials could be
used to modify the corresponding screen-printed carbon ink when
required to achieve higher sensitivity and selectivity. With excel-
lent flexibility and high sensitivity, skin-like pressure sensors have
been extensively used in electronic skin. It is reported that the
breathable pressure sensor with nanofiber membrane can be used
in electronic skin to monitor human physiological signals and
detect spatial pressure distribution [118]. The pressure sensor con-
sists of poly(vinylidene fluoride) nanofiber membranes as the sub-
strate, silver nanowires as the electrode, and thermoplastic
polyurethane nanofiber membrane as the dielectric layer. For
instance, Hu et al. [117] presented graphite nanoplates ink for
screen printing enabled wireless sensor, which could accurately
identify the content of diverse transparent liquids through
machine learning technique, and illustrate the possibility of gra-
phite nanoplates ink to print radiofrequency identification antenna
and wireless sensing system for one-time use, ubiquitous wireless
connections and large-scale applications of internet of things.
Nowadays, the rapid spread of new SARS-CoV-2 coronavirus
around the world triggered COVID-19 pandemic event. Due to
the high infectivity, a speedy and onsite analysis is highly needed
to curb the diffusion of COVID-19. For instance, Arduini et al.
[124] developed a dependable and miniaturized electrochemical
immunosensor to detect SARS-CoV-2. Screen printing electrode
modified by carbon black nanomaterial together with magnetic
beads was used to detect the enzymatic by-product 1-naphthol
for COVID-19. The instrument data has the advantages of stable
consistency, low detection limit, rapid analysis, miniaturization
and portability, as well as easy to operate and non-invasive sam-
pling, which makes the analytical tool an excellent electrochemical
immunoassay method with high sensitivity for the virus detection.
Besides, a stretchable integrated circuit platform has been
demonstrated by screen printing eutectic gallium-indium (EGaIn)
liquid alloy ink onto chemically cross-linked hydrogel substrate
containing numerous hydroxyl groups [125], exhibiting outstand-
ing mechanical robustness and no obvious resistance change even
at an ultrahigh strain of 700%. Further, Shi et al. integrated screen-
printed EGaIn integrated circuit and commercial sensors including
electrocardiogram sensor, thermometer sensor and accelerometer
on polyimine substrate [126], which could realize the effective
detection of heart rate, body temperature and motion state. There-
fore, screen printing technology displays wide application prospect
in wearable and printed micro-sensors.
4. Conclusions and perspectives
In summary, we summarize the recent advances of ink forma-
tion, typical scalable applications, and challenging perspectives of
screen printing for emerging printed microelectronics. It is con-
cluded that the screen printing is undeniably significant and in
urgent demand for flexible, miniaturized and printed electronics.
With the increasingly abundant application requirements, the
screen printing technique is gradually developing towards the
direction of multifunctional integrated microsystems, including
MSCs, MBs and micro-sensors. It should be emphasized that the
most crucial challenge lies in the reasonable design and fabrication
of functional ink with excellent rheological properties. However,
the rheological properties of functional ink are mainly determined
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Journal of Energy Chemistry 63 (2021) 498–513
by the solvents and binders used. To cater for the rapid require-
ment of different electronics applications, the ink needs appropri-
ate viscosity by rationally choosing and deploying the solvents and
binders.
For the screen-printing ink, both organic ink and aqueous ink
need certain special functionality to adapt for the various materials
and applications. Generally, both of them are distinguished from
the most central element of binders dispersing in organic solvent
and water. Hence, much attention should be paid to precisely reg-
ulate the crucial properties of binders, such as superior elasticity
and mechanical strength, high impact toughness, corrosion resis-
tance, adjustable viscoelasticity, excellent thermal and chemical
stability. In addition, the ink of lamellar structural materials (e.g.,
graphene) needs the addition of functional binder to avoid the
re-accumulation and aggregation of lamellar flakes through the
steric hindrance, induced by macromolecules (e.g., PC) and the
electrostatic repulsion between lamellar flakes and binder mole-
cules (e.g., CAB or CMC). However, the functional binders are still
lacking to meet the requirements of printed electronics.
Taking into account the eco-sustainable and environmentally
development, aqueous binders, possessing the crucial merit of
nontoxic and green environmentally, have been drawn consider-
able attention for wearable printed electronics. With the rapid pro-
gressing of printed inks, the bio-binders (e.g., chitosan),
characteristic of biodegradability, biocompatibility, non-toxicity
and optical transparency, are fascinating to accommodate the sub-
strate of skin. So far, the types of binders, especially for the bio-
binders are very limited, which is urgently required for printed
electronics.
First, the printed MBs with in-plane and stacked geometries,
consisting of current collectors, cathode/anode and electrolyte in
between, have been faced several challenges. One urgent challenge
to realize superior electrochemical performance is the printing of
current collectors. Although the expensive metal current collectors
(e.g., Ag, Pt, Cu, Al) have been used for sandwich-like stacked
LIMBs. However, the metal current collectors are difficult to apply
for the in-plane interdigital MBs, due to the metal powder is diffi-
cult to form a stable printable ink. In addition, considering the flex-
ibility and safety, another challenge is to explore high-safe and
mechanically stable electrolytes which can avoid the leak of the
liquid electrolyte and realize the desired flexibility. Screen printing
of printable electrolyte membranes for all-solid-state batteries
would be a good choice. Unfortunately, it is still hard to produce
the printed electrolyte membrane skillfully applied for MBs. In
addition, accurately achieving an adjustable areal loading for
printed MBs remain unsolved. Generally, the speed and pressure
of squeegee directly determined the electrode active materials
loadings, which further influence the match of capacity and
coulombic efficiency of printed electrodes. Hence, it is a precondi-
tion to pursue the desired electrochemical property by accurately
controlling the speed and pressure of screen-printing process.
Second, screen printing is still facing the challenge in the large-
scale production for flexible MSCs. Typically, how to prepare print-
able inks with high viscosity and appropriate shear dilution is still
a thorny problem. In addition, in the process of ink preparation, it
is usually necessary to use inactive additives to prepare electrode
materials ink, which will adversely affect their functional proper-
ties. Therefore, no addition of inactive additives and binders is still
the major focus of screen printing for MSCs as well as MBs in the
future. Besides, screen-printed MSCs need the help of masks to
obtain electrode patterns, and it is still a challenge to produce
high-precision interdigitated electrode patterns.
Third, a variety of new nanomaterials have been recently intro-
duced into the construction of screen-printed electrodes to
improve the performance of the sensor, while the fabrication
strategies of functional printed inks are still limited. At present,
Y. Zhang, Y. Zhu, S. Zheng et al.
most of the studies is focused on adding modified nanomaterials
into the ink to improve its detection sensitivity and develop its
new functions. The use of nanomaterials is considered to be a
promising strategy in the improvement of the reaction rate and
sensor sensitivity. Further, screen printed electrodes are gradually
being used in skin patches and integrated into electronic textiles.
With the development of software for continuous monitoring,
the medical and smart clothing applications of wearable sensors
based on functional nanomaterials will increase significantly, and
go deep into the monitoring of the overall physiological or environ-
mental state, resulting in great demand. Consequently, the durabil-
ity, safety and sensitivity of the printed electronic textiles will be
one of the key issues of future research. In particular, the develop-
ment of screen-printing sensors based on environmentally friendly
materials will be a future focus direction.
Based on the cost-effective and wide range of substrate require-
ments for screen printing, it is widely used in the field of wearable
technology range from the clothing to skin, while how to fabricate
a ‘‘green ink” is still faced a big challenge. In terms of the friendly
environment, the main challenge of ‘‘green ink” lies in the match-
ing of binders and substrates, and the flexibility and stretchability.
In the case of textiles, it is necessary to be very flexible and not
easy to be washed off to accommodate the human daily activities.
However, most of current polymer carriers were used for clothing
printing, such as thermoplastic polyurethane polymers [127] char-
acterized by high transparency, good solubility in various organic
solvents and good mechanical properties, which were served as
the stretchable organic base to achieve high flexibility and stretch-
ability. Furthermore, stretchable electroluminescent structures can
be fabricated using this thermoplastic polyurethane, which can be
directly printed on the textiles by screen printing technology.
Meanwhile, it can be combined with the natural biocompatibility
and biodegradation of biological materials to solve its safety issue.
In addition, printed micro-sensors have high power consumption
in detecting and recording transmission information, and most
devices cannot meet the needs for wearing in a long time. Com-
bined with printed electrochemical energy storage devices such
as MBs and MSCs, a smaller and more durable power supply could
be achieved by printing technique.
With the development of 4D printing in recent years, screen
printing may be directly printed on the substrates of smart mate-
rials in the future, realizing an intelligent design to control the
printed microsystems through certain stimulants, such as water,
temperature, light, and magnetism. Typically, for printed micro-
electronics, it might be possible to control the sensors as well as
the conduction and disconnection of the micro energy storage
device through the changes in body temperature and sweat secre-
tion. In this way, the intelligent characteristics can be extended to
the printed microelectronics systems to realize intelligent control
and comprehensive information communications. Therefore, the
screen printing is a highly promising technology for various indus-
trially applicable printed microelectronics.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgments
This work was financially supported by the National Key R@D
Program of China (2016YFB0100100, 2016YFA0200200), the
National Natural Science Foundation of China (22125903,
51872283, 22075279, 21805273, 22005297, 22005298), the Liao
Ning Revitalization Talents Program (XLYC1807153), the Central
512
Journal of Energy Chemistry 63 (2021) 498–513
Government of Liaoning Province Guides The Funds for Local
Science and Technology Development (2021JH6/10500112), the
Dalian Innovation Support Plan for High Level Talents
(2019RT09), the Dalian National Laboratory For Clean Energy
(DNL), the CAS, DNL Cooperation Fund, CAS (DNL201912,
DNL201915, DNL202016, DNL202019), DICP (DICP ZZBS201708,
DICP ZZBS201802, DICP I2020032), and the China Postdoctoral
Science Foundation (2019M661141, 2020M680995).
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