Materials Today Electronics 6 (2023) 100058

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Materials Today Electronics

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

Review

Formulation of functional materials for inkjet printing: A pathway towards

fully 3D printed electronics
Anil Bastola ♯, Yinfeng He ♯, †, Jisun Im, Geoffrey Rivers, Feiran Wang, Robyn Worsley,
Jonathan S. Austin, Oliver Nelson-Dummett, Ricky D. Wildman *, Richard Hague *,
Christopher J. Tuck *, Lyudmila Turyanska *
Centre for Additive Manufacturing, Faculty of Engineering, University of Nottingham, Nottingham NG7 2RD, United Kingdom

A R T I C L E I N F O A B S T R A C T

Keywords: Inkjet printing offers a facile route for manufacturing the next generation of electronic devices, by combining the
Ink formulation design freedom of additive manufacturing technologies with tuneable properties of functional materials and
Inkjet printing opportunities for their integration into heterostructures. However, to fully realise this potential, the library of
Functional materials
functional materials available for additive manufacturing technologies needs to be expanded. In this review, we
Nanomaterials
Polymers
summarise current developments in ink formulation strategies, approaches for tailoring the functional properties
3D electronics of inks, and multi-material processing. Material – process – property relationships are reviewed for emerging
functional materials, such as polymers, nanomaterials, and composites, with examples of current state-of-the-art
devices. The flexibility of combining inkjet deposition with other existing technologies and a variety of substrates
is also discussed reviewing current trends in electronics and optoelectronics, including wearable electronics,
sensing, and energy applications. The review offers a comprehensive and systematic overview of ink formula­
tions for inkjet deposition of electronic devices, summarising the challenges and perspectives in the advancement
of 3D and multi-functional electronic devices and smart electronics.

1. Introduction parts (e.g., lattice incorporated structures) to enhance the structural

properties such as strength and weight, while the functional AM targets
Additive manufacturing (AM), also known as three-dimensional (3D) on creating parts to perform specific task or functions for examples
printing, is a digital manufacturing process where objects are created in conduct electricity, heat, magnetic field, etc.
a layer-by-layer fashion directly from computer-aided-design (CAD) AM of electronics is one example of functional AM and a rapidly
models. AM has emerged as a disruptive manufacturing process capable growing field as it offers opportunities for the fabrication of low-cost,
of creating highly intricate geometric designs with reduced material lightweight, intricate patterns [8,11]. Compared with conventional
waste compared to traditional manufacturing processes [1–3]. Owing to electronic manufacturing processes such as photolithography [12],
its versatility and cost-effectiveness, AM has been used not only in rapid plating [13] and vacuum deposition [14], AM of electronics can simplify
prototyping but also in large-scale applications to produce structural the device processing by employing direct printing of materials with
end-use parts in various fields, including but not limited to automobile, tailored properties into customized shapes and sizes. amongst a wide
aerospace and civil engineering [4,5]. More recently, the focus of the range of AM techniques, inkjet printing is considered the most promising
research has moved to AM of functional materials relevant for applica­ approach for the deposition of functional materials for electronics, with
tions in areas ranging from biomedicine [6,7] to electronics [8–10]. potential of manufacturing multi-material structures [15,16]. Major
Structural AM typically focuses on creating customised and complex advantages of the inkjet printing technique are its inherent compatibility

* Corresponding authors.
E-mail addresses: ricky.wildman@nottingham.ac.uk (R.D. Wildman), richard.hague@nottingham.ac.uk (R. Hague), christopher.tuck@nottingham.ac.uk
(C.J. Tuck), lyudmila.turyanska@nottingham.ac.uk (L. Turyanska).
♯
Authors contributed equally.
†
Current address: Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute, University of Nottingham Ningbo China, Ningbo 315100,
China.

https://doi.org/10.1016/j.mtelec.2023.100058
Received 29 June 2023; Received in revised form 25 August 2023; Accepted 8 September 2023
Available online 14 September 2023
2772-9494/© 2023 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
A. Bastola et al. Materials Today Electronics 6 (2023) 100058

with almost any substrate of interest, stemming from the additive, metallic material is needed. This can be enabled by comprehensive
non-contact nature of the method, and its versatility to enable the understanding of the approaches to the ink formulations, underpinning
manufacturing of complex structures. This offers the potential to pro­ expansion of AM compatible materials, and by systematic review of the
duce lightweight, flexible, and foldable structures required for the next interconnectivity between the formulation and function in the AM
generation of smart electronics, wearable electronics, biomonitoring process.
systems, medical devices, robotic e-skins, and others [17,18]. In inkjet This review transcends the above-mentioned fields, providing a
printing, the structures are created by depositing droplets of ink through summary of the ink formulating strategy for inkjet deposition of func­
an array of micron-sized nozzles [19,20]. Large-area deposition can be tional materials, manufacturing strategy for co-printing of multiple
achieved with high throughput rates by employing multiple nozzles materials and specific functions achieved. We discuss a range of mate­
[21]. The possibility to use highly tailored inks for electronics such as rials for 3D electronic devices (polymers, nanomaterials and compos­
conductive polymer inks, for example, poly(3,4-ethylene dioxythio­ ites), their functionalities that can be achieved through inkjet
phene) polystyrene sulfonate (PEDOT:PSS) [22], polypyrrole (PPy) deposition, and challenges associated with the performance of inkjet
[23], polyaniline (PANI) [24], and poly-3-hexylthiophene (P3HT) [25] deposited multi-material structures. These concepts are illustrated with
and nanomaterials such as graphene [26], carbon nanotubes (CNTs) examples of state-of-the-art devices, from sensors and detectors to 3D
[27], silver (Ag) [27], gold (Au) [28] and copper (Cu) [29], makes inkjet electronics (Fig. 1). The review focuses on advancements made and
printing one of the best choices for manufacturing of printed electronic remaining challenges of inkjet of electronic devices, including sensors,
devices. energy storage, and fully-3D-printed integrated electronics.
In recent years, there have been significant achievements in the field
of printed electronics through the synergistic utilization of inkjet 2. Functional material inks for inkjet printing
printing and high-performance materials [15,30]. Conductive materials
are the basis for the manufacture of electronic devices and circuits and, Functional material inks suitable for inkjet manufacturing of elec­
as such, conductive inks were amongst the first to be developed for tronics are increasingly expanding with the evolution of new ink for­
printed electronic applications – though largely for two-dimensional mulations and advancement in printhead technologies, where several
electronics. Therefore, there exists a large body of recent work on the inks and printheads are now commercially available. The strategies
deposition of conductive tracks via inkjet printing and their advance­ successfully used for polymeric, nanomaterial, and composite ink ma­
ments, such as the optimisation of conductivity and expansion of sub­ terials for inkjet printing are discussed here. To formulate the inks, a
strate compatibility. Despite growing interest from industry and an number of parameters need to be accounted for, such as ink rheology,
increasing body of research, there remains a limited number of com­ which defines the jetting and jetting stability, as well as contact angle
mercial inkjet printable functional materials available and thus a and coffee ring effects, that control the resolution, surface finish and
step-change in the understanding of the printing process / material uniformity of the printed structure.
properties relationship is needed to truly unleash the potential of AM for
3D electronics.
2.1. Ink formulation strategy
The current approach to printing electronic devices and multi-
material heterostructures requires changing the ink cartridge and/or
The ink consists of various materials such as solvent, particles, and
the substrate during the printing process [31–33]. This allows for the
surfactants. The stability and jettability of the ink, print resolution, and
creation of multi-material planar structures in 2D, and for extending
uniformity of jetted layers are key factors in formulating suitable inks for
them into 3D heterostructures [31]. However, this approach is unable to
inkjet printing [19]. During the inkjet printing process, the ink un­
control ink deposition in a voxel manner, which is necessary for creating
dergoes three different stages: ejection, deposition/spreading, and dry­
functional 3D electronic devices without further steps such as assembly
ing, which all require careful consideration of the ink’s raw materials to
or post-processing. Manufacturing of 3D integrated functional elec­
minimize side effect that cause either printer failure or poor print
tronics such as circuit boards, where the components such as wiring,
quality.
power source, and packaging are all fabricated by a single process is
The key requirements for DOD-based ink formulations include sta­
required. It should be noted that inkjet printing is a forefront technique
bility against aggregation and precipitation, and stability in jetting. The
because its drop-on-demand (DOD) and high-resolution motifs enable
printing stability is governed by the physical properties of the ink, where
voxel-based multi-material printing for fully 3D printed integrated
a Z-value is normally used as an indicator for the jettability of the ink. Z-
electronics. Inkjet printing is a promising method for both 2D planar and
value is a dimensionless inverse of the Ohnesorge (Oh) number:
integrated 3D electronic devices. Integrated 3D printed electronic de­
√̅̅̅̅̅̅̅
vices can be created by combining 2D planar devices, often as hetero­ We η
Oh = 1 /Z = = √̅̅̅̅̅̅̅ (1)
structures. To enable fully 3D printed electronics, where complex 3D Re γ ρa
structures can be directly printed from CAD data, advancemnts in
multimaterial AM technologies and availability of functional material where Re = vρa/η is the Reynolds number, We = v2 ρa/γ is the Weber
formulations need to be achieved. number, ρ is the density, η is the dynamic viscosity, γ is the surface
The primary considerations to achieve fully 3D printed integrated tension, v is the velocity of the fluid, and a is nozzle diameter [38]. The
electronic include: ensuring that the raw functional material is well jettable zone is highlighted in the Fig. 2a. A Z-value between 1 and 10 is
dispersed and loaded in the ink solution to achieve good jettability/ normally considered suitable for inkjet printing.
printability; understanding and optimizing the electronic performance The ink composition also affects jetting, where inks with solid or gel
of the deposited material and interfaces; and efficient post-processing particles are preferred; to prevent nozzle clogging, a commonly used
such as sintering and curing. Therefore, a comprehensive understand­ criterion is that the solid or gel particle size should be below 1/50th of
ing of these factors is crucial, whether in developing heterostructures or the nozzle diameter [20]. The strategy includes the identification of
planar structures, as well as a voxel-based multi-material inkjet printing suitable solvents [41], surfactants [42], and binders [43]. For nano­
(MM-IJ3DP). While MM-IJ3DP offers the possibility to realise complete materials with poor dispersibility, surface functionalisation with organic
3D integrated electronics by accounting for the aforementioned factors materials is used to help improve dispersibility and stability. However, a
just in a single process, yet the ink components and formulation remain post-processing step is often required as the presence of organic mate­
key. Current reviews typically focus on a specific group of materials [34, rials can influence the electrical properties of these layers [44]. The ink
35] or on a specific application [36,37]. However to enable sugnificant viscosity, surface tension and density are optimised to achieve stable
advancement of AM of electronics, dielectric, semiconducting and droplet formation using surfactants, polymers, and solvents. For

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

Fig. 1. Schematic representation of inkjet printing, from ink development and materials, used, and deposition and post-deposition process to examples of
applications.

Fig. 2. Ink droplet formation and deposition. a) The inkjet printable regime is shown in the plot between the Weber number and Reynolds number (adapted from
Ref. [21]). b) Discharge images of inks illustrating the effect of the value of Z (reproduced from Ref. [39]). c) Schematic of the drying process and coffee ring effect.
d) SEM images of printed GO ink droplets on Si/SiO2 substrates after drying at 30 ◦ C showing a transition from a clear coffee ring to a uniformly dried deposit due to
the Marangoni effect as the flake size increases from 500 nm (top image) to 5 mm (bottom image) (reproduced from Ref. [40]). Scale bars are 100 µm in the main
images and 20 µm in the insets.

example, polystyrene [45], ethylene glycol, propylene glycol, and wettability, including the modification of ink formulations [49,50],
glycerol [46] have also been effective in enhancing the viscosity in many substrate coating and surface plasma treatment with oxygen, ultraviolet
ink formulations [31,47,48]. (UV), and ozone (O3) [50,51]. The addition of surfactants, for example,
The droplet deposition and print resolution are governed by ink surfynol [52] and didodecyldiphenyl ether disulfonate [53] is consid­
spreading and drying. For drops deposited at a separation distance, s, the ered to lower the surface energy of the ink and has also been reported to
print resolution on the substrate can be calculated as R = 2,540,0 enhance the ink wetting and pinning. However, the increased wetting
d+s , where
d is the droplet diameter. Several techniques can be applied to enhance can reduce manufacturing resolution, hence optimization of the ink

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

formulation is focused on ensuring the balance between the pinning and ring effect, Matavz et al. [46] developed Ta-Al-Si-alkoxide-based
the feature size. dielectric ink formulations with 2-methoxyethanol as the main solvent
The uniformity of printed structures [54] can be affected by phe­ and highly viscous glycerol or 1,3-propanol as the co-solvent for optimal
nomena such as the coffee ring effect and Marangoni flow [40] (Fig. 2c). viscosity and surface tension. However, a pronounced “coffee-ring” ef­
The coffee ring effect is induced as a result of a combination of contact fect was observed due to the higher volatility of 2-methoxyethanol
line pinning and capillary flow [55], and determine the morphology of compared to the viscous solvents. Consequently, the recirculating Mar­
the final print. To prevent the coffee ring effect, evaporation should be angoni solvent flow exists only at the onset of drying and ceases to exist
driven by flow due to surface tension gradients, known as Marangoni once the 2-methoxyethanol has completely evaporated from the drying
flow [55,56], instead of capillary flow. Marangoni flow can be induced feature. The combination of all three solvents appears to prolong the
by increasing the substrate temperature [57,58], use of high boiling duration of the Marangoni flow, resulting in improved uniformity of
point co-solvents (e.g., diethylene glycol (DEG) and formamide (FA)) dried structures and better device performance. Hu et al. [63] investi­
with a low boiling point main solvent (e.g., water) [59,60]), and by gated isopropanol (IPA)-based alcohol mixtures in various 2D crystal
improving the thermal conductivity between the printed droplet and the inks including graphene, hexagonal boron nitride (h-BN), bismuth
substrate [61]. Hence, to achieve high printing resolution and unifor­ telluride (Bi2Te3), indium selenide (In2Se3), and black phosphorus (BP).
mity, deposition of a solute or ink needs to be optimised by controlling IPA is widely used as a solvent for graphene inks and, recently, for 2D
wettability and Marangoni flow for reproducible production of crystal inks due to its support for a metastable dispersion of the 2D
high-performance printed electronics [56,62]. To eliminate the coffee crystal nanoflakes and its low surface tension for good wetting on

Fig. 3. Overview of inkjet printed conductive polymers. a) Examples of commonly used conductive polymers. b) Summary of charge transfer rates with respect to
chain backbone orientation. (Reproduced from Ref. [72] c) Schematic illustration of aligned p3HT fibres forming based on printing-induced shear-directed crys­
tallization. d) Optical image of the orientated p3HT fibres in the printed line ((c-d) reproduced from Ref. [74]). e) Relative resistance of ink jetted PEDOT:PSS flexible
substrate undergoing bending and f) An example of stable large area PEDOT:PSS ink jetting, 140 serpentine electrodes measuring 10 cm x 6.3 cm without defects
such as bulged lines, missing swaths, missing droplets, or misplaced droplets (e-f reproduced from Ref. [22]).

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

substrates [63,64]. However, the coffee ring effect persists with flow relative to the conductive backbone of the polymer and any local
IPA-based 2D crystal inks. Hu et al. [63] studied the drying mechanism crystalline order (Fig. 3b).
of a binary solvent ink formulation, where Marangoni-enhanced The formulation of conductive polymer inks remains challenging,
spreading inhibits contact line pinning and deforms the droplet shape due to a high degree of chain interaction, resulting in poor solubility and
to naturally suppress the capillary flow that gives rise to the coffee ring high viscosities [75]. The polymers with regularly spaced non-polar side
effect. Liu et al. [65] also demonstrated a binder-free ink composed of chains or groups such as P3HT, PBTTT, polyvinylcarbazole (PVK), poly
black phosphorous and a binary solvent mixture of isopropanol and (N,N’-bis-4-butylphenyl-N,N’-bisphenyl)benzidine (Poly-TPD), or
2-butanol. He et al. [40] suggested that different particle size can also dodecylthiophene (PC12TV12T) can be fully dissolved in non-polar or
influence the coffee ring effect where smaller particles (500 nm) shows chlorinated solvents for use as low-concentration inks (< 1.5 wt.%
less significant coffee ring than the large ones (5 µm) (Fig. 2d). The ink [76]). Poorly soluble polymers are either printed using dispersions of
formulation allows stable jetting, induces recirculating Marangoni flow nanoparticles or gels stabilised by dopant complexes (< 1.5 wt.%, e.g.,
to control the coffee ring effect, and ensures wetting of untreated PEDOT:PSS, PANI, PPY), or are synthesised post-printing through the
substrates. jetting of reactive precursor inks (e.g., PVK, PPy, and PANI). For
multi-phase inks, co-solvents and surfactants are commonly used to
improve their printability and wettability (e.g., gemini surfactants and
2.2. Polymeric inks ethanol in PPy nanodispersion were used to reduce surface tension to
30.8 mN m − 1, compared to 69.8 mN m − 1 without optimisation [23]),
Polymers are of high value in printed electronics, due to their highly while crosslinkers provide post-print stabilisation (e.g. (3-glycidylox­
variable and tailorable properties, including flexibility [66], biocom­ ypropyl)trimethoxysilane (GOPS), divinyl sulfone (DVS), and diac­
patibility [67], electrochemical activity, [68] electrical properties [69], etylene diol (DADOL) [25]).
etc. To deposit polymeric materials, inks are formulated using mono­ In addition to the above modifications to fluid and film mechanics,
mers/copolymers, which are usually polymerised in the AM process or some additives alter the electronic properties of the conductive poly­
in a secondary step. mers through chemical doping and microstructural ordering and are
employed to influence the electrical properties of the polymers [77].
2.2.1. Conductive polymeric inks Additives, such as 1,3,5-trichlorobenzene (TCB) can promote ordering in
To date, a number of conjugated polymers is commonly used for PC12TV12T or polyTPD, [78], resulting in significant improvements in
inkjet deposition, including poly(3,4-ethylenedioxythiophene) poly­ device performance. For example, P3HT crystalline nanofibers used in
styrene sulfonate (PEDOT:PSS), polypyrrole (PPy), polyaniline (PANI) organic field-effect transistors (OFETs) improved 5-fold in drain current
and poly(3-hexylthiophene-2,5-diyl) (P3HT), and poly(2,5-bis(3- and 40-fold in on-off ratio compared to isotropic P3HT [74] (Fig. 3c).
alkylthiophen-2-yl)thieno[3,2-b]-thiophene) (PBTTT) (Fig. 3a). Due to the presence of an ionic bond between the conductive PEDOT and
amongst those, PEDOT:PSS has received significant attention due to its non-conductive PSS molecules, additives with a screening effect are used
ability to form aqueous suspensions and high conductivity (up to 1418 S to achieve favourable microstructures and increase conductivity [71].
cm− 1 [70]). The conductivity is dependant on radical charge transfer To date, dimethyl sulfoxide (DMSO) (1000 S cm− 1 [79]), anionic sur­
along with delocalized electron orbitals of the polymer backbone factants (80 S cm− 1 with the addition of sodium dodecyl sulfonate (SDS)
through hopping (Fig. 3a,b) and materials are oxidised or reduced to [80], 542 S cm− 1 with the addition of dodecylbenzene sulfonic acid
respectively achieve p-type [71] or n-type [72] conduction. The degree (DBSA) were successfully used (Table 1). However, additives that alter
of doping and redox states provide avenues to improve conductivity interchain interactions can also increase viscosity or reduce ink stability,
[73] where charge transfer is dependant on the orientation of current

Table 1
Summary of formulations, post-processing parameters and electrical properties of low dimensional materials and conductive polymers.
Material / solvent Particle size, concentration Processing, Sheet resistance (Rs), conductivity (σ) and mobility (μ) Refs
Post-processing

0D inks
Ag / ethylene glycol 5 - 50 nm 250 ◦ C (curing) Rs = 10 µΩ cm [85]
Ag / water-ethylene glycol < 30 nm 150 ◦ C (curing) Rs = 12.6 µΩ cm [86]
Ag / triethylene glycol monoethyl ether 5 - 8 nm – Rs = 12.6 µΩ cm [87]
Au / xylene 3 nm 180 ◦ C (IR drier) Rs = 16 µΩ cm [88]
Au / petroleum hydrocarbon based non-aromatic solvent 2 − 10 nm 200 ◦ C Rs = 20 µΩ cm [89]
Cu / water-ethylene glycol 126 nm Photonic sintering Rs = 40 µΩ cm [29]
Cu – Photonic sintering Rs = 5 µΩ cm [90]
Ni 3000 nm Photonic sintering Rs = 50,000 µΩ cm [91]
1D and 2D inks
SWCNT-COOH / water 24 μg/mL – Rs = 2 kΩ/sq for 14 layers [92]
SWCNT / water 0.15 mg/mL – Rs = 760 Ω/sq for 12 prints [42]
MWCNT / water – – Rs = 16 kΩ/sq [93]
Graphene / cyclohexanone and terpineol 3.5 mg/mL 950 ◦ C (annealing) Rs = 172.7 kΩ/sq [94]
Graphene / DMF 2 mg/mL 400 ◦ C (annealing) σ = 3400 S/m [95]
rGO / styrene - divinylbenzene - glycerol 0.5 mg/mL Pre reduced Rs = 2.14 kΩ/sq for 12 layers [96]
hBN / water 2 mg/mL 150 ◦ C (annealing) Capacitance 2.0 ± 0.3 nF cm− 2 for ~3 µm layer [97]
Polymeric inks
PEDOT:PSS / water 1.1 wt.% Reactive ink-jetting σ ≤ 800 S cm− 1 [83]
PEDOT:PSS / water 1.1 wt.% – σ = 360 S cm− 1 [25]
0.5–1 wt.% σ = 295 ± 10 S cm− 1
P3HT / chlorobenzene 0.16 wt.% – μ ~ 0.002 to 0.017 cm2V − 1 s − 1
[74]
PBTTT / trichlorobenzene 0.5 wt.% μ ~ 0.05 to 0.1 cm2V − 1 s − 1 [98]
PPy / water 0.3–0.89 M Reactive ink-jetting Rs ~ 25 kΩ/sq on textiles [99]
1
PPy / water various – σ ≤ 4.95 S cm− [23]
PANI / water 0.2–1.2 M Reactive ink-jetting Rs ~ 1 kΩ/sq on textiles [99]

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

hence their concentration has to be optimised to enable jettability [81, additives that crosslink the polymer at available reactive sites (e.g. hy­
82]. For this reason, ionic liquids were found unsuitable for droxyl groups of PVP, crosslinked by (poly(melamine-co-formaldehyde)
single-mixture PEDOT:PSS inks (viscosity > 40 cP at 1 wt.% 1-ethyl-3-­ (PMF); 15 wt.% PVP, 5.8 wt.% PMF in ethanol [111]).
methylimidazolium ethyl sulphate (EMIM:ES), while reaching 900 S
cm− 1 with 2.0 wt.% EMIM:ES [83]), except at very low concentrations 2.3. Nanomaterial-based inks
(less than 0.5 wt.% ionic liquids [84]) in which case the gelation effect
and increased chain mobility also enhanced stretchability. To date, the Nanomaterials, also referred to as low-dimensional materials, have
highest achieved conductivity of an inkjet polymer is 1000 S cm− 1 for great potential in a wide range of functional electronic devices due to
PEDOT:PSS containing 5 wt.% DMSO and 464 S cm− 1 for a their superior electrical, mechanical, thermal, optical, and optoelec­
layer-stablished PEDOT:PSS containing 1 wt.% GOPS [25]. tronic properties. Low dimensional inks for electronics can be catego­
After printing, both thermal annealing and chemical treatment are rized as nanoparticle (0D) inks, which include for example AgNP, AuNP,
commonly used to control and modify the properties of printed layers. CuNP inks [112], nanotube- and nanorod-based (1D) inks, such as
For PEDOT:PSS, significant enhancement of conductivity was achieved CNT-based inks, and 2D nanomaterial inks, which include exfoliated
by immersion in dimethylformamide (DMF), ethylene glycol (EG), layered material inks, such as graphene, hexagonal boron nitride (hBN),
DMSO, or sulfuric acid (723 S cm− 1[100], 1418 S cm− 1[70], 1185 S and transition metal oxides. We note that the dimensionality of the
cm− 1 [101], and 4200 S cm− 1 [102]). The effect of thermal annealing on nanomaterials affects their physical and functional properties, as a result
electrical properties is also dependant on the additives present, with a of quantum confinement effects, and the requirements for ink formula­
small effect observed in pristine PEDOT:PSS (0.15 S cm− 1 uncured, 0.3 S tions are different for nanomaterials with different dimensionality. For
cm− 1 225 ◦ C for 20 min), compared to the significant importance in example, 0D nanoparticles have a layer of capping ligands, that define
glycerol-doped PEDOT:PSS (35 wt.% glycerol, < 1 S cm− 1 uncured, 82.5 their interaction with the solvent. This is not the case for e.g., 2D ma­
S cm− 1 150 ◦ C for 20 min [103]). Recently (2023), highly reliable terials, hence different considerations need to be made to achieve jett­
large-area printing of PEDOT: PSS which is stable under bending, able formulations.
annealing, and exposure to UV or IR light (using the bio-renewable
solvents dihydrolevoglucosenone (cyrene) and glycerol carbonate (GC) 2.3.1. Nanoparticle-based inks
as alternatives to DMSO) for flexible electronics was reported [22] Conductive inks based on metal nanoparticles (NPs) are one major
(Fig. 3e,f). category of printed conductive tracks. Dispersion of metal NPs makes it
Recently, micro-reactive inkjet deposition has been employed to jettable through micron-sized nozzles which can be sintered at lower
bypass inkjet’s limitations and achieve higher performance layers, melting temperatures compared to their bulk counterparts due to their
wherein two low-viscosity precursor inks are combined to synthesize or high surface area-to-volume ratio. They exhibit relatively low electrical
modify the conductive polymer in-situ. This has been demonstrated for resistivities (5–40 µΩ cm, Table 1). Synthesis and ink formulation stra­
sequentially-reacted inkjet-printed PANI (0.11 S cm− 1 [104], 1 kΩ sq− 1 tegies for ligand-functionalised NPs with narrow size distribution have
on textiles [99]), PPy (25 kΩ sq− 1 on textiles [99]). Micro-reactive inkjet been developed to ensure long-term ink stability and jetting quality of
printing of PEDOT:PSS and ionic liquid additive EMIM:ES results in the nanoparticulate conductive inks. To date, AgNP inks are the most
development of a highly conductive PEDOT:PSS microstructure (>50 common [113,114], however different metal NP including gold, copper
cP, 900 S cm− 1 with 2.0 wt.% EMIM:ES, [83]). and nickel are increasingly being investigated (Table 1). Common sur­
face ligands for AgNP inks are poly(acrylic acid) (PAA) [115] and poly
2.2.2. Insulating and dielectric polymeric inks (vinylpyrrolidone) (PVP) [15,85]. These inks offer a low-temperature
Several ink-jettable dielectrics and insulating polymers have been sintering process (< 150 ◦ C), suitable for flexible substrate deposition
demonstrated, including poly-4-vinylphenol (PVP) [105], tripropylene (e.g., PET film), and good cohesion between droplets and improved
glycol diacrylate (TPGDA) [106], photoresist epoxy (brand name SU-8) adhesions to various substrates, including Si/SiO2 wafers, glass, paper
[107], polysiloxane [108], and poly(amic) acid (PAA) (subsequently and polymer films [15,44]. However, anisotropic electrical conductiv­
thermally reacted into polyimide) [109]. The presence of pinhole de­ ity, where vertical conductivity is lower than planar conductivity, is
fects in inkjet dielectric layers is commonly detrimental to device per­ observed due to the presence of organic residues concentrated between
formance [105]. One strategy is to jet photo- or thermally-initiated inks vertically stacked printed layers [27,87,116].
of reactive monomers or short reactive oligomers, such as TPGDA (with AuNP ink is particularly advantageous for bioelectronics that is
2,4‑diethyl-9h-thioxanthen-9-one (DETX) and ethyl 4-(dimethylamino) operational in harsh environments, such as high humidity and salt-rich
benzoate (EDAB) photoinitiator and synergist, respectively [106]) and fluids (e.g., body sweat) due to its chemical stability and biocompati­
diluted epoxides such as SU-8 [107] (reported with a high dielectric bility [28]. Hydrophilic AuNPs protected by a sparse layer of ionic li­
constant of 3, achieved for a 200-nm-thick layer of polysiloxane ther­ gands were prepared for ink formulation by the introduction of a mixed
mally crosslinked at 135 ◦ C [108]). Recently, inkjet printing of poly­ ligand shell comprising an ω-functionalised ionic ligand and a labile
dimethylsiloxane (PDMS) elastomer inks at high concentrations was ligand, with subsequent selective removal of the labile ligands. A sparse
demonstrated for reactive-inkjet, with one ink containing silicone hy­ layer of ligands on AuNPs compared with conventional dense ligands
dride, and second ink containing the silicone oligomer and a Pt catalyst enables destabilisation of the ligand shell at a lower sintering temper­
(both with 60 wt.% in octyl acetate) [66]. Examples of 3D constructs ature (~150 ◦ C) suitable for polymeric substrates without losing the
were reported with individual reactive layers with a thickness of 12.1 critical surface ionic density for dispersibility and increased electrical
μm [66]. conductivity [117]. Introduction of multifunctional thiol, trimethylol­
A second strategy is based on solvent-diluted inks of polymers, such propane tri(3-mercapto propionate), as a cohesion enhancer in the ink
as commercial non-reactive PVP ink (dielectric constant of 3.9 [105]) or formulation of octane thiol-functionalised AuNPs improved the cohe­
self-reacting poly(amic) acid (relative permittivity of 3.41 [109]). For sion and integrity of AuNPs [118].
control of layer thickness in heterostructures, optimisation of the poly­ CuNP ink offers a cost-effective alternative to Au and Ag inks,
mer concentration, droplet spacing, and thermal treatment is effective: however, the susceptibility of Cu to oxidation even before and/or during
PVP with a thickness of ~70 nm was achieved by drying at 90 ◦ C for 10 printing and sintering hinders its application. A precursor-type Cu ink
min followed by 130 ◦ C for 20 min [105], while rapid drying of PAA/­ provides a route to overcome Cu oxidation during ink storage, printing,
polyimide ink at substrate temperatures of 120 ◦ C, 150 ◦ C, and 180 ◦ C and sintering. The ink containing hydrous copper formate with 2-amino-
resulted in a dried layer thickness of 1.0 μm, 1.5 μm, and 2.0 μm, 2-methyl-1-propanol (CuF-AMP) is chemically stable and has a low
respectively [110] Further modifications of these inks are possible with viscosity solution even with high loading, and sintering at 190 ◦ C

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

provides reasonable electrical properties (10.5 µΩ cm) [119]. CuO bundles due to strong van der Waals interactions (~500 eV um-1) and
dispersion ink consisting of water and ethylene glycol coupled with the high aspect ratio (>1000) limits their dispersibility [124]. Noncovalent
pulse-thermal process is another route to eliminate particle oxidation functionalisation of CNTs with polymers (i.e. polymer wrapping) [36]
[29]. and various types of surfactants (e.g., naphthyl-group-based non-ionic
Apart from metal NPs, colloidal semiconductor quantum dots (QDs) surfactant) [42] has emerged as a very effective technique utilising van
and perovskite nanocrystals (NCs) are also attracting significant atten­ der Waals force and π-π interaction to achieve good dispersion for inkjet
tion due to their tuneable optical properties in a wide range of the printing. Soum et al. [35] demonstrated an aqueous CNT ink consisting
electromagnetic spectrum, from visible to short-wave infrared [120]. of multi-walled CNTs (MWCNTs) wrapped with naphthyl-functionalised
QD inks developed in various solvents, including N-methyl-2-­ poly(ethylene glycol) surfactants for a fingerprint sensor device
pyrrolidone (NMP) with 1 wt% of n-butylamine (BTA), provide stable (Fig. 4a-c).
formulations over several days and high-resolution printing of a thin Integration of 1D materials with different composition, such as metal
uniform film [120]. Despite the significant potential, the perovskite nanomaterials, with inkjet printing was explored with Ag nanowires
stability in ambient conditions also remains to be addressed [121]. [122,128], Au nanorods [129] and semiconductor nanorods [130].
Recent research reports demonstrate the enhancement of optical sta­ Conductive silver nanowires have also gained great interest due to their
bility of QDs and perovskite NCs in inkjet printed films, however further high electrical conductivity even at very low concentrations, compared
work is still needed. to AgNP-based conductive inks, and high aspect ratio. However, nozzle
clogging due to flow-induced nanowire alignment when passing through
2.3.2. 1D nanomaterials based inks a nozzle presents challenges for jetting. Patil et al. reported optimal Ag
The field of inkjet printing with 1D material inks is still in its infancy, nanowire length of 1.7 µm for smooth passage of nanowires through a
partially due to challenges with dispersion of 1D materials in inks, as nozzle [123]. Enhanced stability and conductivity can be also achieved
well as controlling their organization in the printed layers [122,123]. by addition of a conductive polymer, polyaniline, as a stabilizing agent.
Amongst 1D materials, carbon nanotubes (CNTs) provide the opportu­ Of particular interest are the opportunities offered by anisotropic
nity for mass-manufacturable, high-performance printed and flexible properties of 1D materials, which can enable ordering and alignment of
large-area electronics due to their impressive mechanical and electrical these nanomaterials within the final structure, as was recently demon­
properties [36]. However, the strong tendency of CNTs to form large strated for Au nanorods [131] and semiconductor CdSe/CdS nanorods

Fig. 4. a) Dispersed CNT ink for inkjet printing and SEM image of CNTs. b) Printed image CNT fingerprint patterns and c) its electrical properties. ((a-c) reproduced
from Ref. [125] d) Schematic illustration of the ECE setup and statistical thickness (a mean thickness of ~1.3 nm) derived from AFM image of 200 ECG flakes on
Si/SiO2. Inset shows the corresponding AFM image of a single ECG flake. e) Images of printed graphene tracks on paper and glass substrates (scale bar 200 μm), and
inkjet printed ‘Graphene’ logo on the paper substrate over an area of 50 mm × 30 mm. f) Printed graphene’s electrical properties on paper (d-f reproduced from
Ref. [126]). g) Schematic illustration of the ink formulation of the aqueous MXene/PEDOT:PSS hybrid ink for inkjet printing of devices and h) transmission electron
microscopy (TEM) image of MXene nanosheets. ((g-h) reproduced from Ref. [127]).

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

[132]. The applications that can be enabled by these developments retained for >80 days by incorporating ascorbate ions as capping- and
range from gas sensing applications [133], to neuromodulation [129] anti-oxidizing agents at ambient temperature. An aqueous inkjet print­
and stretchable electronics [134] . However, there is a limited amount of able MXene/PEDOT:PSS hybrid ink offers remarkable printability with
knowledge with few recent investigations advancing understanding of adjustable viscosity, long-term stability and high volumetric capacitance
strategies for improvement of the functional properties of printed (754 F cm− 3) due to enhanced interlayer contact in the MXene via the
structure [123] and the focus on environmental considerations in PEDOT:PSS layer [127] (Fig. 4g,h).
development of new 1D ink formulations [134].
2.4. Composite inks
2.3.3. 2D nanomaterial-based inks
2D materials are attracting increasing attention due to their unique Within a composite ink, two or more materials are combined to
electrical, mechanical, thermal, and optical properties. They can be produce a multifunctional hybrid possessing tailored properties which
produced using liquid exfoliation of layered crystals to be formulated surpass those existing in the singular, separate components [148].
into inkjet printable inks [135]. Several 2D inks have been reported, Composite multifunctionality is often achieved via a matrix-filler sys­
including conductive graphene [136], semiconductive WS2 [137] and tem, in which the matrix is chosen to match the processing requirements
MoS2 [138], and insulating hexagonal BN (hBN) [97]. The potential to for printing and to ensure the stability and support of micro- or nano­
combine conducting, insulating and semiconducting 2D materials particulate filler materials, whilst these fillers provide functional prop­
within one heterostructure could enable precise tailoring of device erties [149]. The need for flexible and biocompatible electronics, as well
performance with multiple functionalities [31]. Similar to CNT inks, the as reuse of 3D electronics with integrated dielectric and conductive
agglomeration of 2D sheets presents challenges for the inkjet process. materials demand versatile materials that can deliver enhanced perfor­
For graphene oxide (GO) flakes, surface functionalisation with polar mance. Therefore, composite materials have become widely utilised, as
groups enables ink formulation without the need for surfactants [139] they can offer a combination of desirable properties within the single
and printing of ultra-large GO flakes (36 µm diameter) was demon­ material system or device.
strated [140]. Conductive inks containing carbon-based Ag composites are exten­
To formulate graphene inks, flakes produced using supercritical CO2 sively explored, where small amounts of the metallic additive typically
exfoliation [141], lithium tetrahydrofuran expansion [142] and liquid improve conductivity whilst maintaining the low-cost benefits of using
phase exfoliation (LPE) [143] were used. The final properties of printed carbon-based ink. For example, Ag/reduced GO (rGO) inks employing
layers are affected by the flake concentration, printing and curing pro­ simultaneous GO reduction and Ag NP deposition have been demon­
cesses and post-deposition treatment [127]. For example, graphene can strated, with PVP acting as both a reducing agent and stabiliser [150].
be dispersed in aqueous hybrid ink formulation and in environmentally The addition of spherical Ag NPs increased the conductivity of the rGO
benign solvents such as ethanol, with the stabilizing polymer ethyl layer from 800 S m − 1 to 2000 S m − 1 in addition to improving the rGO
cellulose (1:100 graphene/EC) and a mixture of cyclo­ dispersibility. Conductive and transparent films with improved stable
hexanone/terpineol [80] to achieve a high conductivity of 3000 S m − 1 conductivity were demonstrated for rGO composites with Au-decorated
after inkjet printing [26]. Despite several advancements in using liquid Ag nanotriangle platelet additives [151]. The conductive properties of
exfoliated graphene, there are still challenges. The exfoliation method composites comprised of graphene nanoplatelets and reactive Ag pre­
requires a long process time (typically several days) and strongly affects cursors were tuned by post-deposition reduction treatments and Gr
the quality of the flakes, influencing the final properties of printed content adjustment [152].
structures. In addition, the low graphene concentration (< 0.5 mg ml− 1) Achieving conductive layers can be damaging for some flexible and
produced by LPE requires the printing of a large number of layers to stretchable substrates [153], whilst metallic films are prone to cracking
produce functional films [26,41] with a good conductivity (100 S m − 1 and interfacial delamination when subjected to stresses [154].
for ink containing 0.11 g L − 1 annealed at 170 ◦ C [41]). As an alternative Matrix-filler composites, where a flexible and/or stretchable matrix is
route, electrochemical exfoliation (ECE) provides a faster process rendered conductive through the incorporation of fillers to create
(exfoliation achieved in a few minutes) and high-quality graphene flakes percolation pathways are proposed as a potential solution. Ag
(70% single- and bi-layers with large lateral size of 1–10 µm) (Fig. 4d-f) nano-colloids in water-based UV-curable resins were shown to have
[144]. A water-based inkjet printable graphene ink with a high con­ good curability and adhesion to flexible Kapton polyimide substrates
centration (2025 mg mL− 1) was achieved using the ECE method, which [155]. AuNP/PEDOT:PSS core-shell composites have been proposed for
allows stable jetting, quick drying (less than 10 s), good wettability on sinter-free electrodes with increased stability during bending on paper
untreated substrates such as paper and glass with high electrical con­ substrates [156] and PEDOT:PSS has also been combined with
ductivity (3.91 × 104 S m − 1) [144]. small-molecule ionic additives acting as stretchability and electrical
The conduction mechanism in inkjet-printed graphene structures conductivity enhancers [82], and with polyurethane [157]. PDMS-based
arises from inter-flake tunnelling and a recent study showed the packing stretchable electrodes are also commonly used. Nanocomposites based
fraction of the flakes in the printed structure determines the overall on vertically grown CNTs within an inkjet printed PDMS matrix
conductivity [26]. Nevertheless, further studies are needed to under­ demonstrated stable performance as serpentine electrodes (Fig. 5a-c).
stand the effect of flake size and residues of additives and solvents on the Likewise, Ag nanowires have been embedded into PDMS, yet only the
electrical properties of inkjet printed graphene networks. nanowires are inkjet-printed, either via direct-deposition into the liquid
Other 2D layered materials, including hBN [143] and transition elastomer [158] or by the coating of PDMS onto previously-defined Ag
metal dichalcogenides (TMDCs) (MoS2, MoSe2, WS2, WSE2) [145,146], inkjet patterns [159]. The combination of an elastomeric PDMS matrix
have also been produced by liquid-phase exfoliation for inkjet printing with the conductive Ag filler at the ink formulation stage is yet to be
inks. Hexagonal BN is a high-quality insulator and TMDCs are semi­ achieved and could enable the fabrication of fully inkjet-printed, free­
conductors with a desirable bandgap from 1 eV to 2 eV and beyond. The standing, and stretchable electrodes.
inks of these 2D materials are formulated with similar strategies dis­ Composite inks with polymeric matrix and ceramics (e.g., barium
cussed for graphene. Worsley et al. [97] achieved a fully inkjet-printed titanate BaTiO3) filler have been developed, in which the ceramic filler
graphene/hBN/graphene capacitor on a flexible substrate. In searches improves the permittivity and thus increases the polarizability of the
for other 2D crystals with promising mechanical and electrochemical flexible and solution-processable polymer [162]. Barium strontium
characteristics, in addition to electrical characteristics, transition metal titanate (BST) ceramics were surface modified and successfully formu­
carbides (TMCs) have been investigated. Wu et al. [147] demonstrated lated into composite inks with poly(methyl methacrylate) (PMMA)
that the stability of Ti3C2Tx MXene, produced by in situ etching, can be [163] and with flexible poly(ethylene glycol) diacrylate (PEGDA) [164]

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

Fig. 5. a) Cross-section TEM image of the structure incorporating vertically grown CNTs into PDMS for composite stretchable electrodes. b) Photographs of the CNT-
PDMS electrodes with varying designs are shown as prepared and under stretching. c) Resistance changes of the same electrodes in response to strain (left) and after
1000 stretching cycles (right). ((a-c) reproduced from Ref. [160]). d) Schematic and e) photograph of the interdigitated structure of the inkjet-printed nanocomposite
electrodes as employed in supercapacitor devices. f) CV curves measured activated carbon (AC), AC-Bi2O3 and reduced graphene oxide conducting paper (RGCP)
used as a reference, and g) TEM image of the AC-Bi2O3 composites ((d-g) reproduced from Ref. [161]).

to achieve homogeneous printed layers with improved permittivity in increase the surface area available for water adsorption.
comparison to the organic materials alone. Polyvinylidene fluoride Composite materials comprised of a polymeric matrix with CNT
(PVDF) is a dielectric polymer with a large relative permittivity [165] fillers are also increasingly explored as they provide sensitivity to
but with poor solubility [166], and as such, PVDF was combined with chemical environments [177]. Polymer layers can swell in response to
poly(viny alcohol) (PVA) in an all-polymer composite, where the PVA volatile organic compounds, leading to disruption in the conductive
serves to improve the stability as well as breakdown strength of the network of the matrix, altering the distance between the percolating
composite film [167]. Barium titanate (BaTiO3)/epoxy thermoset com­ CNTs and changing the electrical properties. Several ink-jettable
posites were proposed as mechanically-stable ceramic-based layers CNT/polymer composites have been developed [177], including
within inkjet-printed flexible energy harvesters, taking advantage of the CNT-PEDOT:PSS [178] used as an ethanol detecting layer, where the
piezoelectric properties of BaTiO3 [168]. Combined BaTiO3-PVDF ethanol adsorption affects the carrier density within both the CNTs and
composite inks [165] are also used as piezoelectric hybrid materials, the PEDOT:PSS, thus enhancing the sensing performance. Other chem­
however, not all crystalline phases of PVDF can exhibit piezoelectricity, ical sensing composites include CB fillers in a SEBS matrix [179] and a
and in this case, the barium titanate nanofillers act as nucleating agents semiconducting CdSe QD/polymer ink [180].
to encourage and stabilise the formation of the piezoelectric PVDF Furthermore, Gr flakes were added to Ag NP inks, producing a
phase. conductive hybrid material for strain sensor applications on PVA sub­
Composite inks such as Bi2O3/activated carbon (AC) and rGO/MnO2 strates [181]. Gr was also used with iron oxide NPs to fabricate
offer a high surface area for charge storage and a porous structure pre­ inkjet-printed composite strain sensors with magnetic self-healing
senting pathways for the control and diffusion of ions are required in properties on polyurethane substrates [182], and ZnO NPs were added
addition to high conductivity, desired in supercapacitor electrodes to Gr for PDMS-based stretchable strain gauges [183]. In each of these
(Fig. 5d-g). Bi2O3 is of particular interest throughout literature as a filler examples, the use of fillers improves the connectivity between adjacent
within such applications due to its high theoretical capacitance (>1300 graphene flakes, thus enhancing material performance.
F g − 1) [169]. Similarly, rGO/MnO2 composites are frequently used, From this review of the recent work, the opportunities offered by the
with the MnO2 providing high capacitance and the rGO flakes acting as composite material are clear, particularly those arising from control of
large-surface-area conductive binders [170]. Other examples of com­ functional properties enabled by composite composition [148]. How­
posite materials used in this field include MnO2 combined with ever, changes in composition have significant effect on the rheology of
conductive Ag/CNTs [171], rGO added to MoO3 [172], and a combi­ the inks and the jettability [177,178] of the composite materials, hence
nation of Gr-based materials with PANI, including rGO [173], and Gr optimization is required for every iteration of ink composition. From the
hydrogels [174], with the composites in each case showing improve­ review of the literature, the polymer-nanoparticle composites are
ments in electrical properties as well as cycling stability when compared emerging as potentially viable for electronics, where the tunability of
with the individual materials. nanomaterial properties can enable control of function, while requiring
MXene-based composites, combining titanium carbide MXenes and minimal changes to formulation and AM deposition process [149,176,
Ag were formulated [175], in which the MXene provides a large surface 182]
area and hydrophilicity, whilst the Ag increases the conductivity for
sensing applications. Similarly, humidity-sensitive MoS2/PVP compos­ 2.5. Advantages and disadvantages of different functional inks
ite inks were optimised for jetting [176]. In these examples, exposure to
moisture leads to changes in the electrical properties of the composite, To enable inkjet of electronic devices, inks of functional materials
thus providing the sensing mechanism, with the PVP further serving as a with differing properties are needed. Polymer-based, nanomaterial-
stabiliser for the exfoliated MoS2 flakes in the latter case, which in turn based and composite inks, summarised in this review, offer

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

complementary advantages. Polymer-based inks, for instance, offer an explored for printing conductive 3D structures, however further work is
economical option and stable jetting (with minimal nozzle clogging needed to fully understand the opportunities.
compared to filler-based inks), along with good substrate adhesion [22,
66]. However, limited mechanical strength and poor stability of thermal 3.2. Printed optoelectronic devices and sensors
and electrical properties can present challenges [22–25]. In contrast,
nanomaterial-based inks, such as metal nanoparticles, offer advanta­ Optoelectronic devices such as solar cells, and LEDs can be fabricated
geous stable electrical conductivity, strong mechanical properties and on curved and flexible substrates for wearable and healthcare devices.
excellent thermal stability [27–29]. However, high sintering tempera­ However, several challenges such as the deposition of thin uniform
tures (>150 ◦ C [85,89]) add complexity to post processing procedures, layers and the intermixing of materials that often occurs in printed
while high material costs [28] can limit their use. Carbon-based nano­ heterostructures still need to be considered.
materials, such as CNTs and graphene, are lightweight and environ­
mentally benign solutions as electrically conductive materials, however 3.2.1. Solar cells
optimization of the formulations is needed to increase shelf life of the Compared to spin-coating, inkjet printing offers the potential for
device [26,118]. In addition to the aforementioned inks, inkjet printing fabricating larger area solar cells with higher throughput rates and less
of single-crystal films, such as organic semiconductor 2,7-dioctyl[1] material wastage [195]. Inkjet printed solar cells could offer enhanced
benzothieno[3,2-b][1]benzothiophene (C8-BTBT) have been explored. performance, as was demonstrated for conventionally manufactured
Such single crystal materials can be printed in ultrathin and scalable dye-sensitised solar cells, where the conventional platinum (Pt) counter
arrays for high-performance electronic devices [184,185]. electrodes were replaced with cost-effective and flexible inkjet-printed
Composite inks on the other hand can integrate the advantages of graphene [196]. A high power-conversion efficiency (PCE) was ach­
both polymers and nanomaterials but require intricate formulation, and ieved, corresponding to ~70% of the PCE achieved in drop-cast Pt de­
the resulting ink properties can fluctuate significantly based on vices at ~3% of the material cost. The performance of conventional Si
composition, hence further research is needed in this area. Availability solar cells can also be enhanced by surface decoration with an
of inks with different properties can address the needs for specific inkjet-printed anti-reflective porous layer of silicon (Si) QDs. Inkjet
intended application. For instance, polymeric inks are more suitable in printing here enabled low-waste deposition while also allowing for
applications such as wearable electronics, where higher electrical con­ control of the thickness and porosity of the QD film, resulting in a 15%
ductivity is not demanded, or even can be used as a dielectric layer. increase in external quantum efficiency in the 300–400 nm wavelength
Nano-dimensional inks are suitable where enhanced conductivity and range [197].
mechanical robustness is required, such as energy storage devices and In recent years, a record PCE of 22.1% [198] was reported for solar
sensors [87,88]. Carbon based inks could be considered for various cells with a spin-coated perovskite photoactive layer. To achieve scal­
sensing applications including biomedical fields [118,125]. Composite ability and customisation, inkjet-printed perovskite (MAPbI3) photo­
inks present a viable option for harnessing the benefits of both material active layers were inkjet-deposited with the layer thickness controlled
types such as stretchable and flexible electronics [148,177]. by the printing strategy and crystal size tuned by a vacuum annealing
step [199]. The resulting device displayed a PCE of ~11%, comparable
3. Inkjet-printed devices to that achieved in spin-coated devices. Solar cells incorporating
inkjet-printed triple cation Cs0.1(FA0.83MA0.17)0.9Pb(Br0.17I0.83)3) pe­
Inkjet printing provides unique benefits for manufacturing electronic rovskites with improved temperature and moisture stability [200] dis­
devices, allowing for high-performance heterostructures and planar played PCEs up to 12.9% and were shown to withstand temperatures of
structures through drop-on-demand and non-contact deposition. This 80 ◦ C for 120 min with a small decrease in PCE of ~10%. To further
includes the fabrication of thin (< 100 nm) uniform films and tall (> 1 enhance device performance, greater control over the NP crystallisation
mm) structures on various surfaces (e.g., rigid/flexible planar and process is required [200].
conformal) for large-area manufacturing and the next generation of 3D Despite demonstrating lower PCE than perovskite solar cells, organic
electronics. devices offer the benefits of being fully inkjet-printed and are well-suited
for applications in wearable and healthcare electronics [25,201]. In
3.1. High resolution printing of conductive patterns these devices, semi-transparent electrodes were achieved with PEDOT:
PSS and a silver grid [201], and the solar cells were fabricated in an
Achieving high accuracy deposition and high-resolution patterns is ambient atmosphere with an area >1 cm2 and PCE = 4.1%. Fully
paramount for electronics. Significant efforts have been invested into inkjet-printed indium tin oxide (ITO)-free, ultrathin, lightweight organic
optimisation of inkjet printing, particularly printing of conductive pat­ solar cells (Fig. 6c,d) on biocompatible parylene substrates was
terns. Typically, resolution is limited by the size of an individual droplet demonstrated with PCE = 3.6%.
and the positioning accuracy of the printing equipment. A number of
approaches were developed in order to achieve high resolution [186], 3.2.2. LEDs
including optimisation of ink formulation [184,187], altering the wet­ Along with solar cells, the integration of optically active materials
ting properties of the substrate [188], and optimising printing process with the inkjet-printing processes has enabled the fabrication of pho­
and developing strategies for higher pixel packing density [189]. Ink toluminescent films, lasing devices, and LEDs [204,205]. The complex
formulations of metal nanoparticle inks and conductive polymer inks patterns enabled by inkjet deposition make it a particularly attractive
were optimised to control the droplet formation and spreading on the method display applications. Also, the unique and random drying
substrate [22,27,28,76]. Printing strategies have been constantly looked behaviour of each droplet [206] enabled the fabrication of unclonable
at, showing that close arrangement of droplets/pixels by reducing the security labels and full-colour converter films for LEDs using inks of
drop spacing can lead to higher-resolution and high-definition features ZnxCd1− xSeyS1− y QDs encapsulated by NaCl crystals [206]. QD films
[187,190]. Inkjet deposition of soluble sacrificial layers have also shown with optical emission in the red, green, and blue wavelength ranges of
to be advantageous for deposition of high-resolution metal patterns the electromagnetic spectrum were sequentially inkjet-printed onto PET
[191]. Most of the work to date in this area is advantageous for printed (polyethylene terephthalate) substrates to fabricate flexible full-colour
2D electronics, however the challenges associated with achieving high RGB QD@NaCl convertor films for full-colour displays with a pixel
positioning accuracy for multiple layer deposition remains to be fully size of 3.74 ± 0.5 μm [206].
resolved. High-content and high-viscosity conductive inks [192,193] Photoactive materials have also been printed in LED structures. For
and other AM processes, such as multi-photon polymerization [194], are example, a small-molecule organic material 1,1′-(9,9-bis(4-(hexyloxy)

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Fig. 6. a) Schematic diagram of an X-ray detector based on an inkjet-printed perovskite QD photoactive layer and b) temporal dependence of the photocurrent
induced in the device by incident X-rays with response times of ~30 ms. Inset shows a photograph of an array of these photodetectors on a PET substrate ((a-b)
reproduced from Ref. [202]). c) Photograph of an ultralightweight fully inkjet-printed organic solar cell suspended on a soap bubble and d) dependence of the
current density of the solar cell as a function of voltage in dark and light conditions ((c-d) reproduced from Ref. [25]). e) Photograph of a blue organic LED with an
inkjet-printed emissive layer on a flexible transparent substrate and f) the luminance and current density of this device are shown to be superior to that of a reference
device deposited by spin coating ((e-f) reproduced from Ref. [203]).

phenyl)− 9H-fluorene2,7-diyl)dipyrene (PFP-3) was inkjet-printed as an for performing functions such as learning, memorising and visual pro­
emissive layer in an LED to produce large-area light-emitting flexible cessing. There has been a growing interest to develop optical synaptic
patterns (Fig. 6e,f), with a luminance of 800 cd m − 2 at 13 V and devices that mimic the biological synapses using inkjet printing. Gra­
maximum current efficiency of 0.6 cd A − 1 [203]. LEDs were also re­ phene and Ag electrodes were inkjet printed to develop photo-synaptic
ported with an inkjet-printed CdSe/ZnS QD emissive layer [207], where organic field-effect transistors (OFETs) that emulate visual responses
coffee-ring-free and low-roughness QD films were achieved using a to external light [217] with ultralow energy consumption (0.07–34 fJ
mixture of dodecane and cyclohexylbenzene solvents. The fabricated per event). Optoelectronic synaptic transistors based on quantum
LEDs displayed a low turn-on voltage of 2.0 V, a luminance of 12,100 cd dot–metal oxide semiconductor (InP/ZnSe QDs) heterojunctions were
m − 2 at 12 V, and a maximum current efficiency of 4.44 cd A-1. inkjet printed and demonstrated a low power consumption (~5.6 pJ per
More recently, metal halide perovskites have attracted considerable event) for activation [218]. Likewise, inkjet printing of indium-tin-oxide
attention for LED applications due to their high quantum yields and (ITO) synaptic thin-film transistors (TFTs) using solution-processed
tolerance to defects. Hammerschmidt et al. [204] developed a method to high-k zirconium oxide (ZrOx) gate dielectric layer are reported
directly control the crystallisation of inkjet-printed perovskite compos­ [219]. Moreover, the coffee ring effect of ITO during inkjet printing is
ites (MAPbBr3:PEG) and achieved the first inkjet-printed perovskite exploited to develop optoelectronic synaptic transistors [144]; a 10 × 12
emissive layer in an LED. This was performed by blending a PEDOT:PSS coffee-ring structure with a high spatial resolution (142 dpi) with du­
hole injection layer with KCl to create a seeding template for the rable visual detection and memory behaviours were demonstrated.
inkjet-printed perovskite layer. The inclusion of KCl in the PEDOT:PSS Optoelectronic memristors are memory devices that exploit resistive
increased the luminance of the device by a factor of 20, achieving a switching that can be controlled both optically and electronically. Inkjet
maximum luminance of 4000 cd m-2 with a turn-on voltage of 2.5 V. printing is a promising choice to develop resistive switching materials
Charge carrier-transport materials such as ZnO [212], PEDOT:PSS and devices. Various nanoparticle-based inks have been used to develop
[213], PVK [214], and poly-TPD [78] have been also printed, though the memristor devices using inkjet deposition. Metal nanoparticles are one
fabrication of fully inkjet-printed devices remains to be achieved for of the promising choices where the formation of metal oxide can be used
several reasons. As with inorganic solar-cells, LED devices require the to introduce the change in resistance [220,221]. Recently, inkjet-printed
deposition of several layers on top of one another, each with a uniform memristors based on an Ag/WO3-x/Au were reported with a resistive
thickness of ~50 nm [215], which is still challenging via inkjet printing switching ratio of ~100 [222]. Similarly, graphene oxide has been inkjet
and further work on the formulation of inks and their integration with printed to develop metal/insulator/metal memristor devices, although a
the deposition process is needed. Also, the deposition of heterostructures relatively low resistive switching ratio ~ 4 was reported [223]. While
for photodetectors, solar cells, or LEDs can lead to intermixing between this is a fast growing area of research, realistic prospects for inkjet
layers [216], which further affects the ability to control the layer printed devices synaptic devices and memristors can only be achieved
thickness and/or the quality of the interface. with development of comprehensive fundamental understanding of
neural networks. This multidisciplinary research is fast advancing and
3.2.3. Optical synaptic devices and memristors AM can provide an underpinning technology for its exploitation.
The synapse is one of the fundamental elements in the human brain

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

3.2.4. Inkjet printed sensors tunnelling current on the distance between un-sintered nanoparticles,
Ink-jet printing enables the deposition of complex geometries, resulting in a GF of 60 over a wide range of applied strains [208]. The
including deposition onto flexible and curved substrates, often required coffee ring effect was exploited to create 5 μm wide traces of Ag nano­
for sensors. To date, sensing applications have been explored ranging particles and the device performance was reproducible over repeated
from chemical sensing [224] to humidity [225] and strain gauges [226]. loading-unloading cycles (Fig. 7a). A strain gauge functionalised with
For example, a chemical sensor was produced for measurements of heart-muscle cells was found to be responsive to those cells flexing
enzymatic activity [227] where glucose oxidase, lactic oxidase, or mixed (Fig. 7b) [224], reliably detecting changes in the heartbeat in response
lipase/glycerol kinase/L-α-glycerophosphate oxidase inkjet-printed to drugs. It can hence be employed as an implant for real-time moni­
onto PANI hydrogel demonstrated respective sensitivities of 5.03, toring in drug trials.
3.94, and 7.49 μA mM− 1 cm− 2 [228]. An rGO-based sensor could detect Humidity monitoring with gravimetric sensors was achieved with
concentrations of NO2 as low as 500 ppb [229] due to the high sensi­ inkjet-printed GO films [210]. An array of GO capacitors in a
tivity, although with a slow recovery time (> 30 min). Optimization of micro-machined ultrasonic transducer was produced such that water
the sensing layer thickness via inkjet printing strategy can be used to absorption into the graphene changed the resonant frequency of the
balance sensitivity vs response time to improve device operation. The array due to increased mass (Fig. 7c). The high surface-to-volume ratio
sensitivity of low-dimensional materials (e.g., SWCNT, Pd NPs) to the of 2D materials and the presence of hydrophilic edge sites is beneficial
presence of nearby charges was exploited in pH meters, allowing for humidity sensing, and sensors were successfully fabricated using 2D
low-cost, real-time pH monitoring [230]. Also, wearable ‘electronic MoS2 with PVP [176], and titanium MXene functionalised with Ag on a
noses’ were fabricated on PEN substrates for the detection of a variety of flexible PEN substrate [175]. Inkjet-printed interdigitated silver elec­
chemicals, such as ammonia, acetic acid, acetone and ethanol [231]. trodes on paper enabled cost-effective and flexible humidity sensors
High-sensitivity photodetectors are valuable tools for a range of [240], where a change in the resistivity or dielectric constant of paper
applications, from fire detection to advanced communications, and upon water absorption is recorded. The sensitivity of metallic ink layers
several devices have been developed via inkjet printing [162]. One to temperature enables simultaneous temperature and humidity sensing,
method for manufacturing high-performance photodetectors is the sur­ however discriminating between signals due to different factors can be
face decoration of single-layer graphene with inorganic nanomaterials. challenging. A dedicated temperature sensor with high sensitivity (2.23
This has been achieved using HgTe QDs [232] and perovskite nano­ × 10-3 C-1) on a flexible polyimide substrate was demonstrated with Ag
crystals [32] with responsivities up to 106 A/W. These devices had NPs [241], with other examples utilising carbon nanoparticles and
sensitivity ranges tuneable by nanocrystal content and inkjet printing PEDOT:PSS (3.9 mV C-1) [242], or graphene and PEDOT:PSS (0.6 × 10-3
enables the fabrication of different devices on a single silicon (Si) chip. C-1) [243].
This is not possible with other coating techniques such as spin coating
and thus paves the way for advanced sensing devices with multiple 3.3. Inkjet printed energy storage devices
detectors sensitive to different wavelengths on a single chip.
Fully inkjet-printed photodetectors are ideal for wearable electronics Energy storage devices include capacitors, supercapacitors, batte­
as they can be easily manufactured on flexible substrates and person­ ries, and fuel cells. They all require materials with large surface areas,
alized for individuals. To date, fully inkjet-printed photodetectors have which inkjet printing is ideally suited to produce. In this section, we look
been demonstrated with a variety of materials. Ag NPs were deposited at the variety of materials and geometries that have been produced,
onto ZnO films for UV detection [233], where surface plasmons of metal focussing on high-performance or unique designs that cover the range of
NP enhanced the photocurrent of the device, achieving a detectivity of technologies that inkjet printing enables.
1.45 × 1010 Jones at 0.7 mW incident light power. Semi-transparent
PEDOT:PSS electrodes were used in combination with a photoactive 3.3.1. Capacitors and supercapacitors
layer of small organic molecules 7,7′-(4,4-bis(2-ethylhexyl)− 4H-silolo Parallel plate capacitors contain a dielectric material sandwiched
[3,2-b:4,5-b′]dithiophene-2,6-diyl)bis(6-fluoro-4-(5′-hexyl-[2, between two electrodes: ceramic/polymer Ba0.6Sr0.4TiO3 (BST) and poly
2′-bithiophen]− 5-yl) benzo[c][1,2,5] thiadiazole) (T1), [6,6]-phenyl-­ (methyl methacrylate) (PMMA) composites were used with silver elec­
C70-butyric acid methyl ester (PC70BM), and P3HT [234] were used in a trodes [163] and displayed dielectric constants between 20 and 55 at 1
broadband photodetector with both sides photosensitive and an external kHz. Fully-inkjet-printed capacitors consisting of 2D graphene elec­
quantum efficiency above 10%. Fully inkjet-printed photodetectors with trodes were successfully demonstrated with 2D hexagonal boron nitride
tuneable response and high photoresponsivity (up to 102 A/W) were (hBN) as a dielectric material (Fig. 7d) [97]. These devices achieved an
achieved for graphene/perovskite detectors [32]. X-ray detectors were areal capacitance of ~2 nF cm− 2 (Fig. 7e).
fabricated from all-inorganic metal halide perovskite QDs (CsPbBr3) Supercapacitors typically include two electrodes, an active electro­
deposited onto PET and Si/SiO2 substrates with gold counter electrodes lyte, and a separator, with the electrode material being the most
pre-deposited via photolithography [202]. Compared to conventional important component. Supercapacitor electrodes must possess a high
α-Se devices, these devices were 70 times more sensitive with a fast surface area for charge storage and a porous structure to present path­
response time of 30 ms at a low bias voltage of 0.1 V (Fig. 6a, b). ways for the diffusion of ions during the charging/discharging process
Inkjet-printing is scalable to arrays of sensors as well [235]. A grid of [244]. Carbon-based matrices and metal oxide fillers, such as CNT and
sensing capacitors was produced with the layout and resolution of UV-cured triacrylate-polymers [211] (Fig. 7f), were used in fully
industry-standard touchscreens [236] and stable operation at a curva­ inkjet-printed supercapacitors on paper, which displayed an areal
ture as low as 8 mm using poly(methylsiloxane) dielectric, silver con­ capacitance of 100 mF cm− 2 stable over 10,000 charge/discharge cycles.
nectors and flexible PEDOT:PSS electrodes. Inkjet-printed silver Flexible supercapacitors consisting of inkjet-printed rGO and MoO3
electrodes with a size and shape optimised for maximum sensitivity composite electrodes in a poly(vinyl alcohol) (PVA)-H2SO4 solution
were used in capacitors to measure pressure fluctuations [237] and the achieved a high volumetric specific capacitance of 22.5 F cm− 3 at 0.044
precise position of a moveable mirror in a spectrometer [238]. A cm− 3, with a capacitance retention rate of 82% after 10,000
To date, the most common printed mechanical sensors are strain charge-discharge cycles [172]. Similarly, inkjet-printed rGO/MnO2
gauges. A sensitivity, or gauge factor (GF), of 2.77 [239] was demon­ composite supercapacitor electrodes were demonstrated for
strated in inkjet-printed carbon nanotubes by rotating the printing di­ self-powered sensor systems on flexible substrates for wearable wrist­
rection 90◦ between layers to improve film uniformity, whilst a high GF band applications [170]. The printed supercapacitors displayed an areal
of 165 was reported for a graphene-PEDOT:PSS sensor [226]. Novel capacitance of 12.9 mF cm− 2 at 0.12 mA cm− 2, with a capacitance
types of strain gauges exploit the exponential dependence of the retention rate of 80% after 2500 charge-discharge cycles. Several groups

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

Fig. 7. a) The exponential gauge factor of the strain gauge made from the nanowires (blue) and a commercial metal foil strain gauge with a gauge factor of 2 (red) for
comparison (reproduced from Ref. [208]). b) Inkjet-printed graphene strain sensor on a paper substrate under tensile compressive strain. (reproduced from
Ref. [209]) c) Schematic of a cross-section of a single resonance cavity used in a humidity sensor. The inkjet printed graphene layer absorbs water, increasing the
mass of the Si3N4 membrane, and altering the resonant frequency. SiO2 is an insulating layer (reproduced from Ref. [210]). d) a Photograph of a fully inkjet-printed
capacitor with graphene top and bottom electrodes, and an hBN dielectric layer, and e) the capacitance of these devices as a function of the frequency ((d-e)
reproduced from Ref. [97]). f) Inkjet-printed doped passivated graphene flakes (GMP) micro-supercapacitors (MSCs) with printed gold current collectors and GMP
electrodes. From right to left: Photograph of printed on a 4-inch Si wafer and micrographs of a printed device (40 GMP layers) on glass. (reproduced from Ref. [211]).
g) Schematic of ice crystal formation in an ink droplet on the impact on a print-bed with temperature T = − 30 ◦ C and (right image) a highly porous MoS2/GO anode
formed by freeze-drying of the structure (reproduced from Ref. [138]).

report the combination of Gr-based materials with PANI for materials, such as LiFePO4 particles [249] and LiMn1-xFexPO4 [250]. A
inkjet-printed supercapacitor electrodes [173]. PANI-Gr hydrogel com­ freeze-drying process was used to introduce macropores in a MoS2 and
posite electrodes were employed within fully inkjet-printed, free­ rGO composite by printing onto a substrate plate at -30 ◦ C, producing a
standing, macroscopic supercapacitor devices supported by a ‘graphene porous anode for a sodium-ion battery [138] (Fig. 7g). The MoS2 pro­
paper’ which demonstrated a specific capacitance up to 307 F g − 1 at 0.2 vides a layered structure to facilitate ion intercalation and the rGO im­
A g − 1 and maintained 90% capacitance after 1000 charge-discharge proves the conductivity of the printed electrodes. Table 2 shows the
cycles [174]. Inkjet printing was used to deposit pseudocapacitive ad­ specific capacity of the batteries discussed here. To date, each part of a
ditives onto supercapacitor electrodes to enhance capacitance, such as battery has been individually realised by ink-jetting, but an entire bat­
bis-terpyridyl-based molecular cobalt complexes on laser-induced gra­ tery is yet to be achieved, primarily due to the challenge of adequate
phene films separated by a LiCl/PVA solid electrolyte [245]. The areal encapsulation [251]. Also, further improvements in power- and energy
capacitance of the device was enhanced by a factor of 75 to ~0.8 mF densities are needed and can be achieved by enhancing the performance
cm− 2. of materials and the printing resolution for the development of
micro-batteries as well as wearable or even implantable energy storage
3.3.2. Batteries and fuel cells devices in the future.
A battery contains two electrodes – the anode and the cathode – at Fuel cells require a continuous supply of fuel and oxygen to produce
which redox reactions take place to provide current to an external load, power without the need for a recharging process. Similarly to batteries,
which are separated by an electrolyte. Lithium-based batteries provide many of the individual components have been successfully inkjet-
excellent capacity and low density, hence a number of lithium-based printed [258,259]. The first fully-printed hydrogen fuel cell was re­
inks have been formulated to print cathodes [246] and were further ported recently with laser-produced holes in the substrate to allow for
functionalised with allotropes of carbon, such as carbon nanotubes fuel supply [260]. Despite the limited ability of inkjet printing to
(CNT) [247] or carbon black (CB) [248], to improve their conductivity. manufacture the hollow structures required for the fast delivery of re­
The beneficial performance of composite materials as electrodes in actants and removal of waste products from fuel cells, this work
batteries has been demonstrated using CNTs with straight-chain sulphur demonstrated the potential of inkjet printing for the deposition of all
for lithium-sulphur batteries [247], and PEDOT:PSS with silicon nano­ active layers required.
particles (Si NP) and CB for lithium-ion batteries [248]. These electrodes
offer high theoretical capacity, reduced cracking, enhanced cycling 3.4. Fully inkjet printed integrated electronics toward 3D electronics
stability, improved conductivity, and mechanical and chemical stability,
and PEDOT:PSS acts as a binder to prevent damage due to the volume The primary benefit of inkjet printing is its ability to facilitate the
expansion typically seen upon Li-ion insertion. multi-material inkjet-based 3D printing (MM-IJ3DP) process, which
Porosity can also be improved by using naturally microporous incorporates multiple DOD printheads within a single machine. This

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

Table 2
Commercial and state-of-the-art inkjet printed devices and their performance parameters. Material deposited using inkjet printing are indicated with tick (✓).
Commercial and state of art Materials Properties/Performance Ref.
technology or devices Printed Specific Capacity (Cp), Discharge rate (Q), No of cycles (N)
and notable features

Batteries Anode: Si NPs/PEDOT:PSS ✓ Cp = 2500 mAhg− 1, Q = 0.1 C, N = 1 [248]

Cathode: Li foil - Cp = 1000 mAhg− 1, Q = 0.1 C, N = 1000
Electrolyte: 1 M LiPF6 -
Anode: Li foil - Cp = 800 mAhg− 1, Q = 0.1 C, N = 100 [247]
Cathode: Li-S/S@SWNT ✓
Electrolyte: 1 M LiCF3SO3 -
Anode: Li foil - Cp = 800 mAhg− 1, Q = 9 C, N = 100 [250]
Cathode: LiMn0.21Fe0.79PO4@C Electrolyte: 1 M LiPF6 ✓ Cp = 150.2 mAhg− 1, Q = 10 C, N = 1000 Cp: 108.4 mAhg− 1,
- Q = 100 C, N = 1000
Anode: Ag ✓ Cp = 70 mAhg− 1, Q = 0.04 C, N = NA [252]
Cathode: Ag ✓
Electrolyte: 10 M KOH/ZnO -
Anode: MoS2/graphene aerogel ✓ Cp = 429 mAhg− 1, Q = C/3.3, N = 10 [138]
Cathode: Sodium -
Electrolyte: 1 M NaClO4 -
Anode: Li4Ti5O12 - Cp = 60 mAhg− 1, Q = 0.1 C, N = 100 [253]
Cathode: LiFePO4 -
Electrolyte: Silica ionogel ✓

PCBs Substrates: PET, PI - Min trace width: 150 µm [254]

from Elephantech Inks: Ag NPs ✓ Build dimension: 180 × 270 mm,1 layer
Deposition: Thermal inkjet
Ag NPs as nucleation points for Cu deposition
PCBs Substrates: PET, ITO, glass, PI - Trace width: 70 µm [255]
from PV Nanocell Inks: Ag, Au, Cu NPs ✓ Build dimension: 427 × 365 mm,1 layer
Up to 10 inks simultaneously
Deposition: Piezo inkjet; speed 1.1 m2/hr
PCBs from BotFactory Substrates: FR4 epoxy, Kapton film, and other flexible - Trace width: 200 µm [256]
and rigid substrates - Build dimension: 117 × 152 mm, 4 layers
Inks: Ag NPs, dielectric ✓ Deposition: Thermal inkjet; Integrated with the pick-and-
place installation system
PCBs from Nano Dimension Substrates: FR4 epoxy, Si wafer, Cu foil, polycarbonate, - Trace width: 80 µm [257]
Kapton film - Build dimension: 160 × 160, 3 layers
Inks: Ag NPs, acrylate-urethane ✓ Deposition: Piezo inkjet

integration allows users to simultaneously print different materials at a flexible substrates. The organic semiconductor P3HT was blended with
minute (pico-litre) scale. Additional advantages include the co- the insulating amorphous polystyrene (PS) for protective encapsulation
deposition of various materials (such as conductive and dielectric and printed as a channel material in FETs, which demonstrated maximum
inks), easy scalability, direct printing onto the desired substrate, and the field-effect mobility and on/off current ratio of 0.02 cm2 V − 1 s − 1 and
production of metamaterials in a non-contact printing method. These 106, respectively. The structure of the printed blend films can be tuned by
factors collectively make inkjet printing a practical method for the composition of the solvent mixture [265]. Sholz et al. [263] fabricated
achieving 3D electronics [261]. The main electronic components and fully-inkjet-printed metal-oxide (indium-oxide) thin-film transistors
other accessories such as the wiring, power source, and packaging are all (TFTs) on ITO substrates with PEDOT:PSS top-gate electrodes. Inherent
to be fabricated by a single process, which could be enabled by inkjet random variations of the surface roughness of each inkjet-printed device
printing. To fully realise the integrated 3D electronics, multiple mate­ were exploited to generate unique identifiers for data security applica­
rials need to be printed together. Multimaterial electronics printing can tions [263].
be realised either by changing the ink cartridge or substrate or The combination of a graphene active channel, silver electrodes, and
combining various processes. This method has been widely reported to an hBN dielectric layer was used to realise fully-inkjet-printed FETs [26]
(
develop vertical 3D heterostructures and planner 2D structures with Fig. 8b). Depth profiling and 3D mapping revealed that the printed
various inks. This section reviews advancements in the fabrication of graphene layer was non-homogeneous and large intermixing of layers
fully inkjet-printed transistors and printed circuit boards (PCBs) and 3D was present due to the inkjet printing deposition method (Fig. 8c). To
inkjet-printed electronics. Further, we discuss the requirements and account for this, the charge transport model was developed to include
progress in multi-material inkjet 3D printing (MM-IJ3DP) towards fully quantum tunnelling between graphene flakes and percolation dynamics
3D-printed integrated electronics. [26]. This revealed that the electrical properties of the device are
strongly influenced by the packing fraction of graphene flakes and by
3.4.1. Transistors complex electron trajectories that traverse several printed layers, illus­
Fully inkjet-printed transistors have been a major focus of study in trating the complex transport dynamics of inkjet-printed electronic de­
recent years [262,263]. Field effect transistors (FETs) were demonstrated vices. At low gate voltages (<5 V), the aforementioned FETs displayed
in a vertical heterostructure configuration, where inkjet printing enabled field-effect mobilities of 25 cm2 (V s)− 1 [26] and 91 cm2 (V s)− 1 [143].
the simultaneous deposition of the silver source and drain electrodes with Further miniaturization of inkjet-printed transistors is still needed, but
an isolated organic semiconductor layer (Poly[2,5-bis(alkyl)pyrrolo[3, the opportunities for customisation and integration with other processes
4-c]pyrrole-1,4-(2H,5H)‑dione-alt-5,5′- di(thiophen-2-yl)− 2,2′-(E)− make these devices attractive for different applications [263].
2-(2-(thiophen-2-yl)vinyl)-thiophene] (PDVT-8)) [264]. An array of these It should be noted that fabricating a single transistor device can be
devices was demonstrated with favourable stability and ultrashort chan­ expanded to create 3D electronics. For example, fully inkjet 3D printed
nel lengths with current densities exceeding 6 mA cm− 2 on both rigid and monolithic integrated flexible transistors were developed by staking

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A. Bastola et al. Materials Today Electronics 6 (2023) 100058

Fig. 8. a) An example of 3D electronics, optical images and schematic diagram of device assembly. The sensor node is comprised of an assembly of a 3D-printed
functional package, circuit board, and air capacitor (reproduced from Ref. [266]). b-c) Multi-material fully inkjet printed heterostructure or planner devices to­
wards 3D electronics, b) fully inkjet-printed planner graphene/hBN FET device (reproduced from Ref. [26]) and c) fully inkjet printed perovskite nano­
crystals/graphene heterostructure photodetector device (reproduced from Ref. [32]). d) Voxel-based MM-IJ3DP approach. Schematic illustrating deposition of
functional materials as voxels (50 ~ 100 µm) into complex 3D structures (left). The spatial distribution of each material voxel is designed to produce a target structure
(middle). Photograph of a PCB device with spatially distributed spiral conductive tracks manufactured by MM-IJ3DP (reproduced from Ref. [87]) (right).

single-gate and dual-gate organic transistors [267]. Similarly, fully enable multi-layer printing for greater circuit density. BotFactory
inkjet printed 3D integrated circuits (ICs) based on a 3D complementary (Table 2) achieved this by coating each layer of circuitry with a
organic field-effect transistor were achieved by vertically stacking a dielectric mixture of UV-curable acrylates and urethanes, allowing gaps
p-type OFET over an n-type OFET with a shared gate joining the two for vias to join up to 4 layers together. A catalyst-based approach was
transistors [268,269]. In addition, taking advantage of the flexibility of used to form two-sided PCBs on a paper substrate, including printed vias
polymeric substrates, various flexible and wearable electronic TFT de­ [275]. Here, silver nanoparticles were inkjet-printed as catalysts for
vices with excellent electrical characteristics and mechanical stability electroless copper deposition, with the depth of metallisation optimised
have been fully inkjet printed on ultra-flexible polymer films [270]. AM by the amount of deposited ink. Alternatively, vias were printed only
has already enable significant benefits for fabrication of thin film and using Ag nanoparticle ink, however, circuit failure occurred when the
organic FETs with high resolution [271–273]. PCB was folded due to the poor adhesion [276].
Recently, Nano Dimension achieved accurate deposition of silver at
3.4.2. Printed circuit boards desired places within its build volume, with the dielectric acting as a
Fully printed circuit boards (PCBs) can be produced using inkjet support matrix and an electrical insulator. Although limited to a 3 mm
printing of the conductive traces, offering highly customisable and low- build height, this is sufficient to print native componentry, such as in­
waste manufacturing. Several companies such as Elephantech and PV ductors or antennas, within the multi-layered PCB [257]. Free-standing
Nanocell (see Table 2), have already adopted inkjet processes for PCB and encapsulated vertical silver interconnects were produced with
fabrication. Recently, highly flexible PCBs were printed on a stretched heights up to 10 mm high and an aspect ratio approaching 50 [261],
PDMS substrate to induce wrinkles in the Ag traces when the strain is potentially enabling inkjet printing of space-efficient PCBs [261].
released [274] and demonstrated spiral conductive tracks manufactured
by MM-IJ3DP (reproduced from Ref. [87]) (Fig. 8c). The next step is to

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3.4.3. Antennas 4. Concluding remarks and outlook

Manufacturing of antennas requires flexibility of deposition to pro­
duce the geometries needed for designed bandwidth, gain, and direc­ Inkjet printing is an important AM technique in the field of elec­
tionality [277]. Several two-dimensional antennas have been tronics due to a number of appealing advantages, such as a high degree
inkjet-printed using Ag NP inks and graphene-based inks [278,279]. of fabrication flexibility and the possibility to use various functional
More recently, 3D deposition was demonstrated by the PolyJet system inks. Electronic devices including but not limited to sensors, transistors,
from Stratasys, where selective UV-curing of polymer precursor inks capacitors, displays, PCBs, solar cells, and batteries have been success­
enabled the inkjet-printing of complex 3-dimensional polymeric struc­ fully developed via inkjet printing. The functional inks for inkjet print­
tures [280], which can be can be functionalised by conformal printing ing can be broadly categorized as conductive polymer inks, low
onto them. A printed two-turn helix attached to a Fresnel lens was dimensional inks, and composite inks. This review has comprehensively
functionalised with inkjet-printed silver NPs onto the outer edge of the highlighted a wide range of functional inks and their formulation stra­
helix [281], resulting in a fully inkjet-printed, 3-dimensional antenna, tegies, the inkjet printing process for both single-material and multi-
with the lens providing 4.6 dB of gain. material inks, and inkjet-printed electronic devices within the current
Exploiting flexible electronics can also give pseudo-three- state-of-the-art.
dimensional printing by printing on a substrate in the shape of a Inkjet printing has been extensively used to create 2D planar elec­
cube’s net and then folding it up to give a three-dimensional shape for tronic devices. Recently, increasing attention is focused on
improved antenna design as well as space to fit internal electronics. manufacturing of fully inkjet-printed 3D integrated electronic devices
Kimionis et al. [282] inkjet-printed silver patches on a polymer sub­ [267–269]. 2D planar printing is faster compared to 3D printing and
strate, which was first printed separately with the PolyJet system. The allows for rapid prototyping applications. This means that the func­
fold-lines were made from a shape-memory polymer capable of tionality of the deposited materials can be studied before they are used
self-assembling and subtly changing shape under temperature fluctua­ in 3D devices. It is important to note that 3D printed integrated elec­
tions. The antenna had characteristics modified by its shape, so – com­ tronic devices are not created directly from 3D CAD data, however,
bined with some electronics packed into the internal void to harness RF recent development in multi-material AM technologies and growing
energy through the antenna – it could act as a wireless temperature availability of functional materials could offer opportunities for fully 3D
sensor, potentially as part of a large network. In other reports, the as­ printed electronics.
sembly of multiple functional components within one structure are Although an increasing number of articles reports the fabrication of
demonstrated (Fig. 8a). Origami-like antennae printed on paper, after fully inkjet-printed electronics, taking advantage of the technique in
folding and sealing, were shown to float and be waterproof. Other ex­ terms of the scalability, the adaptable digital device design, and the low-
amples combine antennae, sensors, PCBs and air capacitors. While a few waste additive nature of the manufacture, a particular lack of free-
examples have emerged in the literature, there is still a significant need standing, 3D inkjet-printed devices is notable. Several works discussed
for the development of truly 3D inkjet-printed architectures to realise above rely on use of supporting substrate, with devices deposited on top
complete 3D inkjet-printed electronics. in the form of 2D circuits. However, as reported in recent studies, the
integrated 3D electronics employs printed layer as a substrate for the
3.4.4. Multi-material inkjet 3D printing (MM-IJ3DP) for 3D electronics formation of heterostructures or 3D electronic configurations
Although there has been significant progress in fully printed elec­ [267–269]. Saleh et al. [87] report circuitry deposited within 3D poly­
tronics, such as multi-material heterostructures or planar structures, meric structures using a single MJ system, with Ag NP and TPGDA inks
printing does not offer the voxel-wise control which will enable 3D in­ jetted in the same process via a piezo-based inkjet system and cured in
tegrated electronics. Further developments are constantly required to real-time with a UV light source. This is a promising approach to the
enable the manufacture of 3D electronics, due to the complexity of the realisation of 3D printed objects with embedded electronic functional­
circuits in 3D and the need for the assembly of different components. ities, yet each of the inks is jetted separately from individual cartridges.
Therefore, there is a strong interest in voxel-wise multi-material inkjet Additional challenges in realisation of 3D electronics are
3D printing for 3D electronics. Multi-material inkjet-based 3D printing process-related, where the micro-scale resolution of the deposited
(MM-IJ3DP) integrates multiple DOD printheads within one machine, structure presents obstacles for fabrication of miniaturised devices. This
which enables the co-printing of different materials at a pico-litre scale requires further technological advancements of the hardware as well as
(Fig. 8d), offering a voxel-control, unlike its 2D counterpart. understanding of and optimization of the printing strategies. Also, the
There are several challenges facing the fabrication of 3D electronics need for post-processing to achieve the function can bring undesirable
through MM-IJ3DP. Different inks require different energy sources to complexity to the manufacturing process.
either functionalise or cure them, such as infrared (IR) or ultraviolet A potential future direction within inkjet-printed electronic appli­
(UV) light for solidification (Fig. 8d), or intense pulsed light (IPL) for cations should focus on the inclusion of electronically active fillers into
sintering [51,52]. In the solidification process, the entire structure is structurally supportive (polymeric) matrices for 3D printed devices
exposed, and sample damage could occur and should be considered in fabricated entirely through MMIJ3DP and cured in real-time. Such an
the formulating process. For example, to sinter metallic nanoparticle approach exploits both the multifunctionality of the ink materials and
inks, elevated temperatures (120–150 ◦ C) are required [53], which can the multifunctional MMIJ3DP process. This will require optimisation of
be detrimental to polymeric substrates underneath [54]. To date, this the filler content to find a balance between the final electronic proper­
challenge is addressed by optimizing ink formulations and the solidifi­ ties and the initial jettability of the ink, where a higher solid loading
cation process [40]. For example, inkjet-printable polyimide was re­ typically leads to increased percolation pathways or improved perfor­
ported which was thermally stable up to 400 ◦ C [55] and UV light was mance yet challenges the viscosity limitations of the inkjet printing
used to replace the thermal sintering of silver nanoparticles in dielectric process. Furthermore, the effect of filler content on composite curability
polymeric materials [56]. The interface in MM-IJ3DP between different must be addressed, notably in the case of light-based post-processing
materials is another crucial factor that should be considered when methods, where excessive fillers may obscure light penetration and
formulating the inks [26]. The preferable scenario is an interface, where hinder effective curing. Saleh et al. [15] combined magnetic iron oxide
the two distinct materials either inter-diffuse into each other in a with a UV-curable resin, demonstrating successful material jetting and
controlled way or have a covalent bonding, preventing delamination or real-time curing of 3D structures, along with their electromagnetic
early failure [6]. characterisation. Likewise, functional inks incorporating 0D, 1D and 2D
fillers with a wide variety of electronic properties, should be developed
and deposited in different combinations via MMIJ3DP for future

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demonstrations of fully inkjet-printed 3D devices that can be deposited [11] Y. Khan, A. Thielens, S. Muin, J. Ting, C. Baumbauer, A.C. Arias, Adv. Mater. 32
(2020), 1905279.
and post-processed in a scalable manner. Furthermore, future research
[12] H. Lee, C. Bae, L.T. Duy, I. Sohn, D. Kim, Y. Song, Y. Kim, N. Lee, Adv. Mater. 28
and development should also be focused on improving the printed res­ (2016) 3069–3077.
olution, low sensitivity of printed devices, and limited range towards [13] S. Faraji, F.N. Ani, Renew. Sustain. Energy Rev. 42 (2015) 823–834.
fully 3D printed functional devices. [14] C. Chen, H. Kang, S. Hsiao, P. Yang, K. Chiang, H. Lin, Adv. Mater. 26 (2014)
6647–6652.
Although there are several challenges for MM-IJ3DP as a production [15] E. Saleh, P. Woolliams, B. Clarke, A. Gregory, S. Greedy, C. Smartt, R. Wildman,
tool for electronics, we are also seeing a growing interest as well as I. Ashcroft, R. Hague, P. Dickens, C. Tuck, Addit. Manuf. 13 (2017) 143–148.
impressive studies that are targeting these challenges. Predictive [16] Y. He, B. Begines, G.F. Trindade, M. Abdi, J.F. Dubern, E. Prina, A.L. Hook, G.
Choong, J. Ledesma, C.J. Tuck, F.R.A.J. Rose, R. Hague, C.J. Roberts, D. de
modelling has been introduced as a solution to help the user predict Focatiis, I.A. Ashcroft, P. Williams, D.J. Irvine, M.R. Alexander, R.D. Wildman,
whether a failure could happen with a chosen combination of materials ChemRxiv (2020).
as well as whether the chosen set of solidification processes will lead to [17] J. Lemarchand, N. Bridonneau, N. Battaglini, F. Carn, G. Mattana, B. Piro, S. Zrig,
V. Noël, Angew. Chemie Int. Ed. 61 (2022), e202200166.
sample cracking or delamination by residual stresses or thermal [18] D.F. Fernandes, C. Majidi, M. Tavakoli, J. Mater. Chem. C 7 (2019) 14035–14068.
expansion. Tim et al. [283] presented a finite element analysis method [19] B. Derby, Annu. Rev. Mater. Res. 40 (2010) 395–414.
to analyse and predict product quality using acrylic and silver nano­ [20] A. Sajedi-Moghaddam, E. Rahmanian, N. Naseri, ACS Appl. Mater. Interfaces 12
(2020) 34487–34504.
particles as an example of multi-material inkjet-printed electronics. [21] B. Derby, N. Reis, MRS Bull. 28 (2003) 815–818.
Professor Bailey from the University of Greenwich introduced an [22] G. Rivers, J.S. Austin, Y. He, A. Thompson, N. Gilani, N. Roberts, P. Zhao, C.
indicative manufacturing process where an artificial intelligence (AI) J. Tuck, R.J.M. Hague, R.D. Wildman, L. Turyanska, Addit. Manuf. 66 (2023),
103452.
monitoring unit was introduced to help improve the quality of manu­
[23] B. Weng, R. Shepherd, J. Chen, G.G. Wallace, J. Mater. Chem. 21 (2011)
factured products [283]. Inkbit3D also presented their latest machine 1918–1924.
vision and AI technology that allows the machine to in-line monitor [24] N.T. Brannelly, A.J. Killard, Electroanalysis 29 (2017) 162–171.
parts shrinkage and distortions, provide feedback to the machine and [25] E. Bihar, D. Corzo, T.C. Hidalgo, D. Rosas-Villalva, K.N. Salama, S. Inal, D. Baran,
Adv. Mater. Technol. 5 (2020), 2000226.
compensate for these variations. All these modelling and in-line moni­ [26] B. Wang, L. Kari, Polym. 13 (2021).
toring technologies can largely improve the manufacturing accuracy and [27] G.F. Trindade, F. Wang, J. Im, Y. He, A. Balogh, D. Scurr, I. Gilmore, M. Tiddia,
production yield for MM-IJ3DP for printed electronics [283]. E. Saleh, D. Pervan, L. Turyanska, C.J. Tuck, R. Wildman, R. Hague, C.J. Roberts,
Commun. Mater. 2 (2021) 47.
The inkjet technology still has a way to go in some areas. A better [28] J. Im, G.F. Trindade, T.T. Quach, A. Sohaib, F. Wang, J. Austin, L. Turyanska, C.
resolution will be needed to break into the microdevices market in a J. Roberts, R. Wildman, R. Hague, C. Tuck, A.C.S. Appl, Nano Mater. 5 (2022)
major way, and some materials are unavailable to print, whilst others 6708–6716.
[29] M.S. Rager, T. Aytug, G.M. Veith, P. Joshi, ACS Appl. Mater. Interfaces 8 (2016)
still fall behind in performance compared to other production processes. 2441–2448.
The largest obstacle is still the limitations of going into the third [30] V. Beedasy, P.J. Smith, Materials (Basel) 13 (2020) 704.
dimension, although work from academia and industry alike are [31] D. McManus, S. Vranic, F. Withers, V. Sanchez-Romaguera, M. Macucci, H. Yang,
R. Sorrentino, K. Parvez, S.K. Son, G. Iannaccone, K. Kostarelos, G. Fiori,
certainly looking to break through soon, be it vertical interconnects, C. Casiraghi, Nat. Nanotechnol. 12 (2017) 343–350.
high-density PCBs, or folded structures. [32] J.S. Austin, N.D. Cottam, C. Zhang, F. Wang, J.H. Gosling, O. Nelson-Dummet, T.
S.S. James, P.H. Beton, G.F. Trindade, Y. Zhou, Nanoscale 15 (2023) 2134–2142.
[33] O. Song, D. Rhee, J. Kim, Y. Jeon, V. Mazánek, A. Söll, Y.A. Kwon, J.H. Cho, Y.
Declaration of Competing Interest H. Kim, Z. Sofer, J. Kang, NPJ 2D Mater. Appl. 6 (2022) 64.
[34] S. Chung, K. Cho, T. Lee, Adv. Sci. 6 (2019), 1801445.
The author(s) declared no potential conflicts of interest with respect [35] L. Nayak, S. Mohanty, S.K. Nayak, A. Ramadoss, J. Mater. Chem. C 7 (2019)
8771–8795.
to the research, authorship, and/or publication of this article.
[36] K. Yan, J. Li, L. Pan, Y. Shi, APL Mater. 8 (2020), 120705.
[37] G.L. Goh, H. Zhang, T.H. Chong, W.Y. Yeong, Adv. Electron. Mater. 7 (2021),
Data availability 2100445.
[38] Z. Zhou, L.Ruiz Cantu, X. Chen, M.R. Alexander, C.J. Roberts, R. Hague, C. Tuck,
D. Irvine, R. Wildman, Addit. Manuf. 29 (2019), 100792.
No data was used for the research described in the article. [39] R. Noguera, M. Lejeune, T. Chartier, J. Eur. Ceram. Soc. 25 (2005) 2055–2059.
[40] P. He, B. Derby, Adv. Mater. Interfaces 4 (2017), 1700944.
[41] F. Torrisi, T. Hasan, W. Wu, Z. Sun, A. Lombardo, T.S. Kulmala, G.W. Hsieh,
S. Jung, F. Bonaccorso, P.J. Paul, ACS Nano 6 (2012) 2992–3006.
Acknowledgements [42] O.S. Kwon, H. Kim, H. Ko, J. Lee, B. Lee, C.H. Jung, J.H. Choi, K. Shin, Carbon N.
Y. 58 (2013) 116–127.
This work was funded by the Engineering and Physical Sciences [43] F. Scuratti, J.M. Salazar-Rios, A. Luzio, S. Kowalski, S. Allard, S. Jung, U. Scherf,
M.A. Loi, M. Caironi, Adv. Funct. Mater. 31 (2021), 2006895.
Research Council Programme Grant [grant number EP/P031684/1]. [44] I.J. Fernandes, A.F. Aroche, A. Schuck, P. Lamberty, C.R. Peter, W. Hasenkamp,
T. Rocha, Sci. Rep. 10 (2020) 8878.
References [45] C.A. Lamont, T.M. Eggenhuisen, M.J.J. Coenen, T.W.L. Slaats, R. Andriessen,
P. Groen, Org. Electron. 17 (2015) 107–114.
[46] A. Matavz, R.C. Frunza, A. Drnovsek, V. Bobnar, B. Malic, J. Mater. Chem. C 4
[1] S.A.M. Tofail, E.P. Koumoulos, A. Bandyopadhyay, S. Bose, L. O’Donoghue,
(2016) 5634–5641.
C. Charitidis, Mater. Today 21 (2018) 22–37.
[47] S. Jeong, H.C. Song, W.W. Lee, S.S. Lee, Y. Choi, W. Son, E.D. Kim, C.H. Paik, S.
[2] J.Y. Lee, J. An, C.K. Chua, Appl. Mater. Today 7 (2017) 120–133.
H. Oh, B.H. Ryu, Langmuir 27 (2011) 3144–3149.
[3] X. Zheng, H. Lee, T.H. Weisgraber, M. Shusteff, J. DeOtte, E.B. Duoss, J.D. Kuntz,
[48] P. Yang, L. Zhang, dong J. Kang, R. Strahl, T. Kraus, Adv. Opt. Mater. 8 (2020),
M.M. Biener, Q. Ge, J.A. Jackson, Science (80-.) 344 (2014) 1373–1377.
1901429.
[4] Y.W.D. Tay, B. Panda, S.C. Paul, N.A. Noor Mohamed, M.J. Tan, K.F. Leong,
[49] Y.S. Goo, Y.I. Lee, N. Kim, K.J. Lee, B. Yoo, S.J. Hong, J.D. Kim, Y.H. Choa, Surf.
Virtual Phys. Prototyp. 12 (2017) 261–276.
Coatings Technol. 205 (2010) S369–S372.
[5] A. Uriondo, M. Esperon-Miguez, S. Perinpanayagam, Proc. Inst. Mech. Eng. Part G
[50] S.H. Lee, Y.J. Cho, J. Electr. Eng. Technol. 7 (2012) 91–96.
J. Aerosp. Eng. 229 (2015) 2132–2147.
[51] B.K. Lok, X. Hu, in: 2010 12th Electron. Packag. Technol. Conf., IEEE, 2010,
[6] Y. He, R. Foralosso, G.F. Trindade, A. Ilchev, L. Ruiz-Cantu, E.A. Clark, S. Khaled,
pp. 240–245.
R.J.M. Hague, C.J. Tuck, F.R.A.J. Rose, Adv. Ther. 3 (2020), 1900187.
[52] P. Wilson, C. Lekakou, J. Watts, in: 2012 12th IEEE Int. Conf. Nanotechnol, IEEE,
[7] T. Ahmadraji, L. Gonzalez-Macia, T. Ritvonen, A. Willert, S. Ylimaula,
2012, pp. 1–6.
D. Donaghy, S. Tuurala, M. Suhonen, D. Smart, A. Morrin, V. Efremov, R.
[53] A. Kamyshny, M. Ben-Moshe, S. Aviezer, S. Magdassi, Macromol. Rapid Commun.
R. Baumann, M. Raja, A. Kemppainen, A.J. Killard, Anal. Chem. 89 (2017)
26 (2005) 281–288.
7447–7454.
[54] J.H. Kim, S. Il Ahn, J.H. Kim, W.C. Zin, Langmuir 23 (2007) 6163–6169.
[8] A. Kamyshny, S. Magdassi, Chem. Soc. Rev. 48 (2019) 1712–1740.
[55] R.D. Deegan, O. Bakajin, T.F. Dupont, G. Huber, S.R. Nagel, T.A. Witten, Nature
[9] L. Yang, H. Hu, A. Scholz, F. Feist, G. Cadilha Marques, S. Kraus, N.
389 (1997) 827–829.
M. Bojanowski, E. Blasco, C. Barner-Kowollik, J. Aghassi-Hagmann, M. Wegener,
[56] H. Hu, R.G. Larson, J. Phys. Chem. B 110 (2006) 7090–7094.
Nat. Commun. 14 (2023) 1103.
[57] K.Y. Shin, S.H. Lee, J.H. Oh, J. Micromech. Microeng. 21 (2011) 45012.
[10] A. Willert, F.Z. Tabary, T. Zubkova, P.E. Santangelo, M. Romagnoli, R.
[58] Z. Xiong, C. Liu, in: 18th Eur. Microelectron. Packag. Conf., IEEE, 2011, pp. 1–4.
R. Baumann, Int. J. Hydrogen Energy 47 (2022) 20973–20986.

17
A. Bastola et al. Materials Today Electronics 6 (2023) 100058

[59] J. Park, J. Moon, Langmuir 22 (2006) 3506–3513. [101] T.R. Chou, S.H. Chen, Y. Te Chiang, Y.T. Lin, C.Y. Chao, J. Mater. Chem. C 3
[60] D. Kim, S. Jeong, B.K. Park, J. Moon, Appl. Phys. Lett. 89 (2006), 264101. (2015) 3760–3766.
[61] W.D. Ristenpart, P.G. Kim, C. Domingues, J. Wan, H.A. Stone, Phys. Rev. Lett. 99 [102] N. Kim, S. Kee, S.H. Lee, B.H. Lee, Y.H. Kahng, Y.R. Jo, B.J. Kim, K. Lee, Adv.
(2007), 234502. Mater. 26 (2014) 2268–2272.
[62] M. Kuang, J. Wang, B. Bao, F. Li, L. Wang, L. Jiang, Y. Song, Adv. Opt. Mater. 2 [103] Z. Xiong, C. Liu, Org. Electron. 13 (2012) 1532–1540.
(2013) 34–38. [104] L. Pan, G. Yu, D. Zhai, H.R. Lee, W. Zhao, N. Liu, H. Wang, B.C.K. Tee, Y. Shi,
[63] G. Hu, L. Yang, Z. Yang, Y. Wang, X. Jin, J. Dai, Q. Wu, S. Liu, X. Zhu, X. Wang, T. Y. Cui, Z. Bao, Proc. Natl. Acad. Sci. U. S. A. 109 (2012) 9287–9292.
C. Wu, R.C.T. Howe, T. Albrow-Owen, L.W.T. Ng, Q. Yang, L.G. Occhipinti, R. [105] N. Graddage, T.Y. Chu, H. Ding, C. Py, A. Dadvand, Y. Tao, Org. Electron. 29
I. Woodward, E.J.R. Kelleher, Z. Sun, X. Huang, M. Zhang, C.D. Bain, T. Hasan, (2016) 114–119.
Sci. Adv. 6 (2020) eaba5029. [106] Y. He, F. Zhang, E. Saleh, J. Vaithilingam, N. Aboulkhair, B. Begines, C.J. Tuck, R.
[64] S. Abdolhosseinzadeh, X. Jiang, H. Zhang, J. Qiu, C.(John) Zhang, Mater. Today J.M. Hague, I.A. Ashcroft, R.D. Wildman, Addit. Manuf. 16 (2017) 153–161.
(2021). [107] A. Moya, E. Sowade, F.J. del Campo, K.Y. Mitra, E. Ramon, R. Villa, R.
[65] H. Liu, W. Xu, W. Tan, X. Zhu, J. Wang, J. Peng, Y. Cao, J. Colloid Interface Sci. R. Baumann, G. Gabriel, Org. Electron. 39 (2016) 168–176.
465 (2016) 106–111. [108] A. Dadvand, J. Lu, C. Py, T.Y. Chu, R. Movileanu, Y. Tao, Org. Electron. 30 (2016)
[66] C. Sturgess, C.J. Tuck, I.A. Ashcroft, R.D. Wildman, J. Mater. Chem. C 5 (2017) 213–218.
9733–9745. [109] J. Zhang, A. Chaudhari, H. Wang, J. Manuf. Process. 45 (2019) 710–719.
[67] I. Louzao, B. Koch, V. Taresco, L. Ruiz-Cantu, D.J. Irvine, C.J. Roberts, C. Tuck, [110] F. Zhang, E. Saleh, J. Vaithilingam, Y. Li, C.J. Tuck, R.J.M. Hague, R.D. Wildman,
C. Alexander, R. Hague, R. Wildman, M.R. Alexander, ACS Appl. Mater. Interfaces Y. He, Addit. Manuf. 25 (2019) 477–484.
10 (2018) 6841–6848. [111] B.J. Kang, C.K. Lee, J.H. Oh, Microelectron. Eng. 97 (2012) 251–254.
[68] T. Beduk, E. Bihar, S.G. Surya, A.N. Castillo, S. Inal, K.N. Salama, Sensors [112] J. Szczech, C. Megaridis, J. Zhang, D. Gamota, Microscale Thermophys. Eng. 8
Actuators B Chem. 306 (2020), 127539. (2004) 327–339.
[69] M.N. Gueye, A. Carella, N. Massonnet, E. Yvenou, S. Brenet, J. Faure-Vincent, [113] J. Yang, P. He, B. Derby, ACS Appl. Mater. Interfaces 14 (2022) 39601–39609.
S. Pouget, F. Rieutord, H. Okuno, A. Benayad, R. Demadrille, J.P. Simonato, [114] J. Vaithilingam, E. Saleh, L. Körner, R.D. Wildman, R.J.M. Hague, R.K. Leach, C.
Chem. Mater. 28 (2016) 3462–3468. J. Tuck, Mater. Des. 139 (2018) 81–88.
[70] Y.H. Kim, C. Sachse, M.L. MacHala, C. May, L. Müller-Meskamp, K. Leo, Adv. [115] W. Shen, X. Zhang, Q. Huang, Q. Xu, W. Song, Nanoscale 6 (2014) 1622–1628.
Funct. Mater. 21 (2011) 1076–1081. [116] H.H. Lee, K.S. Chou, K.C. Huang, Nanotechnology 16 (2005) 2436.
[71] M.N. Gueye, A. Carella, J. Faure-Vincent, R. Demadrille, J.P. Simonato, Prog. [117] B.T. Anto, S. Sivaramakrishnan, L.L. Chua, P. K.H.Ho, Adv. Funct. Mater. 20
Mater. Sci. 108 (2020), 100616. (2010) 296–303.
[72] R. Balint, N.J. Cassidy, S.H. Cartmell, Acta Biomater. 10 (2014) 2341–2353. [118] K.T. Park, Y.S. Cho, I. Jeong, D. Jang, H. Cho, Y. Choi, T. Lee, Y. Ko, J. Choi, S.
[73] X. Li, Z. Liu, Z. Zhou, H. Gao, G. Liang, D. Rauber, C.W.M. Kay, P. Zhang, A.C. Y. Hong, M.W. Oh, S. Chung, C.R. Park, H. Kim, Adv. Energy Mater. 12 (2022),
S. Appl, Polym. Mater. 2021 (2020) 98–103. 2200256.
[74] T. Rödlmeier, T. Marszalek, M. Held, S. Beck, C. Müller, R. Eckstein, A.J. Morfa, [119] Y. Farraj, M. Grouchko, S. Magdassi, Chem. Commun. 51 (2015) 1587–1590.
R. Lovrincic, A. Pucci, U. Lemmer, J. Zaumseil, W. Pisula, G. Hernandez-Sosa, [120] R. Sliz, M. Lejay, J.Z. Fan, M.J. Choi, S. Kinge, S. Hoogland, T. Fabritius, F.
Chem. Mater. 29 (2017) 10150–10158. P. Garciá de Arquer, E.H. Sargent, ACS Nano 13 (2019) 11988–11995.
[75] R. Kroon, D.A. Mengistie, D. Kiefer, J. Hynynen, J.D. Ryan, L. Yu, C. Müller, [121] J.H. Yoo, S.G. Jeong, S.H. Choi, S. Bin Kwon, Y.H. Song, D.H. Yoon, Ceram. Int. 47
Chem. Soc. Rev. 45 (2016) 6147–6164. (2021) 6041–6048.
[76] A. Giuri, S. Masi, A. Listorti, G. Gigli, S. Colella, C. Esposito Corcione, A. Rizzo, [122] S. Wang, X. Wu, J. Lu, Z. Luo, H. Xie, X. Zhang, K. Lin, Y. Wang, Nanomaterials 12
Nano Energy 54 (2018) 400–408. (2022) 842.
[77] H. Yuk, B. Lu, S. Lin, K. Qu, J. Xu, J. Luo, X. Zhao, Nat. Commun. 11 (2020) 1–8. [123] P. Patil, S. Patil, P. Kate, A.A. Kulkarni, Nanoscale Adv. 3 (2021) 240–248.
[78] A. Giuri, E. Saleh, A. Listorti, S. Colella, A. Rizzo, C. Tuck, C.Esposito Corcione, [124] W.B. Liu, S. Pei, J. Du, B. Liu, L. Gao, Y. Su, C. Liu, H.M. Cheng, Adv. Funct.
Nanomaterials 9 (2019) 582. Mater. 21 (2011) 2330–2337.
[79] A. De Girolamo Del Mauro, R. Diana, I.A. Grimaldi, F. Loffredo, P. Morvillo, [125] V. Soum, S. Park, A.I. Brilian, Y. Kim, M.Y. Ryu, T. Brazell, F.J. Burpo, K.
F. Villani, C. Minarini, Polym. Compos. 34 (2013) 1493–1499. K. Parker, O.S. Kwon, K. Shin, ACS Omega 4 (2019) 8626–8631.
[80] B. Fan, X. Mei, J. Ouyang, Macromolecules 41 (2008) 5971–5973. [126] K. Parvez, R. Worsley, A. Alieva, A. Felten, C. Casiraghi, Carbon N. Y. 149 (2019)
[81] H. Ling, R. Chen, Q. Huang, F. Shen, Y. Wang, X. Wang, Green Chem. 22 (2020) 213–221.
3208–3215. [127] J. Ma, S. Zheng, Y. Cao, Y. Zhu, P. Das, H. Wang, Y. Liu, J. Wang, L. Chi, S.
[82] Y. Wang, C. Zhu, R. Pfattner, H. Yan, L. Jin, S. Chen, F. Molina-Lopez, F. Lissel, (Frank) Liu, Z.S. Wu, Adv. Energy Mater. 11 (2021), 2100746.
J. Liu, N.I. Rabiah, Z. Chen, J.W. Chung, C. Linder, M.F. Toney, B. Murmann, [128] E. Marzbanrad, H.H. Khaligh, (2023).
Z. Bao, Sci. Adv. (2017) 3. [129] H. Kang, G.H. Lee, H. Jung, J.W. Lee, Y. Nam, ACS Nano 12 (2018) 1128–1138.
[83] M.Y. Teo, N. Ravichandran, N. Kim, S. Kee, L. Stuart, K.C. Aw, J. Stringer, ACS [130] S. Halivni, S. Shemesh, N. Waiskopf, Y. Vinetsky, S. Magdassi, U. Banin,
Appl. Mater. Interfaces 11 (2019) 37069–37076. Nanoscale 7 (2015) 19193–19200.
[84] X. Fan, W. Nie, H. Tsai, N. Wang, H. Huang, Y. Cheng, R. Wen, L. Ma, F. Yan, [131] K. Saito, K. McGehee, K. Manabe, Y. Norikane, RSC Adv. 11 (2021) 22376–22380.
Y. Xia, Adv. Sci. 6 (2019), 1900813. [132] S.K. Gupta, M.F. Prodanov, W. Zhang, V.V. Vashchenko, T. Dudka, A.L. Rogach,
[85] B.Y. Ahn, S.B. Walker, S.C. Slimmer, A. Russo, A. Gupta, S. Kranz, E.B. Duoss, T. A.K. Srivastava, Nanoscale 11 (2019) 20837–20846.
F. Malkowski, J.A. Lewis, J. Vis. Exp. JoVE (2011). [133] J. Lin, M. Kilani, G. Mao, Adv. Mater. Technol. (2023), 2202038.
[86] Q. Huang, W. Shen, Q. Xu, R. Tan, W. Song, Mater. Chem. Phys. 147 (2014) [134] R. Madhavan, J. Mater. Sci. Mater. Electron. 33 (2022) 3465–3484.
550–556. [135] D.J. Finn, M. Lotya, G. Cunningham, R.J. Smith, D. McCloskey, J.F. Donegan, J.
[87] E. Saleh, F. Zhang, Y. He, J. Vaithilingam, J.L. Fernandez, R. Wildman, N. Coleman, J. Mater. Chem. C 2 (2014) 925–932.
I. Ashcroft, R. Hague, P. Dickens, C. Tuck, Adv. Mater. Technol. 2 (2017), [136] Y. Hernandez, V. Nicolosi, M. Lotya, F.M. Blighe, Z. Sun, S. De, I.T. McGovern,
1700134. B. Holland, M. Byrne, Y.K. Gun’Ko, J.J. Boland, P. Niraj, G. Duesberg,
[88] A. Maattanen, P. Ihalainen, P. Pulkkinen, S. Wang, H. Tenhu, J. Peltonen, ACS S. Krishnamurthy, R. Goodhue, J. Hutchison, V. Scardaci, A.C. Ferrari, J.
Appl. Mater. Interfaces 4 (2012) 955–964. N. Coleman, Nat. Nanotechnol. 3 (2008) 563–568.
[89] Y. Khan, F.J. Pavinatto, M.C. Lin, A. Liao, S.L. Swisher, K. Mann, V. Subramanian, [137] J.A. Desai, S. Mazumder, R.F. Hossain, A.B. Kaul, J. Vac. Sci. Technol. B
M.M. Maharbiz, A.C. Arias, Adv. Funct. Mater. 26 (2016) 1004–1013. Nanotechnol. Microelectron. Mater. Process. Meas. Phenom. 38 (2020) 52201.
[90] Y. Ren, J. Virkki, L. Sydänheimo, L. Ukkonen, Electron. Lett. 50 (2014) [138] E. Brown, P. Yan, H. Tekik, A. Elangovan, J. Wang, D. Lin, J. Li, Mater. Des. 170
1504–1505. (2019), 107689.
[91] B.N. Altay, V.S. Turkani, A. Pekarovicova, P.D. Fleming, M.Z. Atashbar, [139] B. Dai, L. Fu, L. Liao, N. Liu, K. Yan, Y. Chen, Z. Liu, Nano Res. 4 (2011) 434–439.
M. Bolduc, S.G. Cloutier, Sci. Rep. 11 (2021) 1–12. [140] P. He, B. Derby, 2D Mater. 4 (2017) 21021.
[92] E. Gracia-Espino, G. Sala, F. Pino, N. Halonen, J. Luomahaara, J. Mäklin, G. Toth, [141] Y. Gao, W. Shi, W. Wang, Y. Leng, Y. Zhao, Ind. Eng. Chem. Res. 53 (2014)
K. Kordás, H. Jantunen, M. Terrones, ACS Nano 4 (2010) 3318–3324. 16777–16784.
[93] S. Azoubel, S. Shemesh, S. Magdassi, Nanotechnology 23 (2012), 344003. [142] K. Arapov, R. Abbel, H. Friedrich, Faraday Discuss 173 (2014) 323–336.
[94] Q. He, S.R. Das, N.T. Garland, D. Jing, J.A. Hondred, A.A. Cargill, S. Ding, [143] T. Carey, S. Cacovich, G. Divitini, jiesheng Ren, A. Mansouri, J.M. Kim, C. Wang,
C. Karunakaran, J.C. Claussen, ACS Appl. Mater. Interfaces 9 (2017) C. Ducati, R. Sordan, F. Torrisi, Nat. Commun. 8 (2017) 1202.
12719–12727. [144] K. Liang, R. Wang, H. Ren, D. Li, Y. Tang, Y. Wang, Y. Chen, C. Song, F. Li, G. Liu,
[95] J. Li, F. Ye, S. Vaziri, M. Muhammed, M.C. Lemme, M. Östling, Adv. Mater. 25 H. Wang, W.R. Leow, B. Zhu, Adv. Opt. Mater. 10 (2022), 2201754.
(2013) 3985–3992. [145] J. Li, M.M. Naiini, S. Vaziri, M.C. Lemme, M. Östling, Adv. Funct. Mater. 24
[96] N. Karim, S. Afroj, A. Malandraki, S. Butterworth, C. Beach, M. Rigout, K. (2014) 6524–6531.
S. Novoselov, A.J. Casson, S.G. Yeates, J. Mater. Chem. C 5 (2017) 11640–11648. [146] A.G. Kelly, T. Hallam, C. Backes, A. Harvey, A.S. Esmaeily, I. Godwin, J. Coelho,
[97] R. Worsley, L. Pimpolari, D. McManus, N. Ge, R. Ionescu, J.A. Wittkopf, A. Alieva, V. Nicolosi, J. Lauth, A. Kulkarni, S. Kinge, L.D.A. Siebbeles, G.S. Duesberg, J.
G. Basso, M. MacUcci, G. Iannaccone, K.S. Novoselov, H. Holder, G. Fiori, N. Coleman, Science (80-.) 356 (2017) 69–73.
C. Casiraghi, ACS Nano 13 (2019) 54–60. [147] C.W. Wu, B. Unnikrishnan, I.W.P. Chen, S.G. Harroun, H.T. Chang, C.C. Huang,
[98] M. Baklar, P.H. Wöbkenberg, D. Sparrowe, M. Gonçalves, I. McCulloch, Energy Storage Mater. 25 (2020) 563–571.
M. Heeney, T. Anthopoulos, N. Stingelin, J. Mater. Chem. 20 (2010) 1927. [148] H. Abdolmaleki, A.B. Haugen, K.B. Buhl, K. Daasbjerg, S. Agarwala, Adv. Sci. 10
[99] Z. Stempien, T. Rybicki, E. Rybicki, M. Kozanecki, M.I. Szynkowska, Synth. Met. (2023), 2205942.
202 (2015) 49–62. [149] E. Saleh, 3D 4D Print, Polym. Nanocomposite Mater. (2020) 505–525.
[100] J. Dong, G. Portale, Adv. Mater. Interfaces 7 (2020), 2000641.

18
A. Bastola et al. Materials Today Electronics 6 (2023) 100058

[150] W. Zhang, E. Bi, M. Li, L. Gao, Colloids Surfaces A Physicochem. Eng. Asp. 490 [200] F. Mathies, H. Eggers, B.S. Richards, G. Hernandez-Sosa, U. Lemmer, U.
(2016) 232–240. W. Paetzold, ACS Appl. Energy Mater. 1 (2018) 1834–1839.
[151] L. Li, M. Gao, Y. Guo, J. Sun, Y. Li, F. Li, Y. Song, Y. Li, J. Mater. Chem. C 5 (2017) [201] T.M. Eggenhuisen, Y. Galagan, A.F.K.V. Biezemans, T.M.W.L. Slaats, W.
2800–2806. P. Voorthuijzen, S. Kommeren, S. Shanmugam, J.P. Teunissen, A. Hadipour, W.J.
[152] J. Zhao, M. Song, C. Wen, S. Majee, D. Yang, B. Wu, S.L. Zhang, Z.B. Zhang, H. Verhees, S.C. Veenstra, M.J.J. Coenen, J. Gilot, R. Andriessen, W.A. Groen,
J. Micromech. Microeng. 28 (2018). J. Mater. Chem. A 3 (2015) 7255–7262.
[153] J. Brenneman, D.Z. Tansel, G.K. Fedder, R. Panat, Extrem. Mech. Lett. 43 (2021). [202] J. Liu, B. Shabbir, C. Wang, T. Wan, Q. Ou, P. Yu, A. Tadich, X. Jiao, D. Chu, D. Qi,
[154] K.D. Harris, A.L. Elias, H.J. Chung, J. Mater. Sci. (2015) 2771–2805. D. Li, R. Kan, Y. Huang, Y. Dong, J. Jasieniak, Y. Zhang, Q. Bao, Adv. Mater.
[155] D. Zhai, T. Zhang, J. Guo, X. Fang, J. Wei, Colloids Surfaces A Physicochem, Eng. (2019) 31.
Asp. 424 (2013) 1–9. [203] L. Zhou, L. Yang, M. Yu, Y. Jiang, C.F. Liu, W.Y. Lai, W. Huang, ACS Appl. Mater.
[156] D.J. Kang, Y. Juttke, L. Gonzalez-Garcia, A. Escudero, M. Haft, T. Kraus, Small 16 Interfaces 9 (2017) 40533–40540.
(2020), e2000928. [204] F. Hermerschmidt, F. Mathies, V.R.F. Schröder, C. Rehermann, N.Z. Morales, E.
[157] K. Kim, M. Jung, B. Kim, J. Kim, K. Shin, O.S. Kwon, S. Jeon, Nano Energy 41 L. Unger, E.J.W. List-Kratochvil, Mater. Horizons 7 (2020) 1773–1781.
(2017) 301–307. [205] G. Hu, T. Albrow-Owen, X. Jin, A. Ali, Y. Hu, R.C.T. Howe, K. Shehzad, Z. Yang,
[158] K.N. Al-Milaji, Q. Huang, Z. Li, T.N. Ng, H. Zhao, ACS Appl. Electron. Mater. 2 X. Zhu, R.I. Woodward, T.C. Wu, H. Jussila, J. Bin Wu, P. Peng, P.H. Tan, Z. Sun,
(2020) 3289–3298. E.J.R. Kelleher, M. Zhang, Y. Xu, T. Hasan, Nat. Commun. 8 (2017).
[159] Q. Huang, K.N. Al-Milaji, H. Zhao, A.C.S. Appl, Nano Mater. 1 (2018) 4528–4536. [206] S.J. Ho, H.C. Hsu, C.W. Yeh, H.S. Chen, ACS Appl. Mater. Interfaces 12 (2020)
[160] S. Hong, J. Lee, K. Do, M. Lee, J.H. Kim, S. Lee, D.H. Kim, Adv. Funct. Mater. 33346–33351.
(2017) 27. [207] Y. Liu, F. Li, Z. Xu, C. Zheng, T. Guo, X. Xie, L. Qian, D. Fu, X. Yan, ACS Appl.
[161] P. Sundriyal, S. Bhattacharya, A.C.S. Appl, Energy Mater. 2 (2019) 1876–1890. Mater. Interfaces 9 (2017) 25506–25512.
[162] Y. Wang, M. Yao, R. Ma, Q. Yuan, D. Yang, B. Cui, C. Ma, M. Liu, D. Hu, J. Mater. [208] Z. Zhang, T. Si, Sensors Actuators A Phys. 264 (2017) 188–194.
Chem. A 8 (2020) 884–917. [209] C. Casiraghi, M. Macucci, K. Parvez, R. Worsley, Y. Shin, F. Bronte, C. Borri,
[163] M. Mikolajek, T. Reinheimer, N. Bohn, C. Kohler, M.J. Hoffmann, J.R. Binder, Sci. M. Paggi, G. Fiori, Carbon N. Y. 129 (2018) 462–467.
Rep. 9 (2019). [210] Z. Zheng, N. Kim, W.S. Wong, J.T.W. Yeow, Sensors Actuators B Chem. 327
[164] T. Reinheimer, R. Azmi, J.R. Binder, ACS Appl. Mater. Interfaces 12 (2020) (2021), 128920.
2974–2982. [211] S. Sollami Delekta, M.M. Laurila, M. Mäntysalo, J. Li, Nano-Micro Lett. 12 (2020)
[165] H. Abdolmaleki, S. Agarwala, Polym. 12 (2020). 40.
[166] G. Zapsas, Y. Patil, Y. Gnanou, B. Ameduri, N. Hadjichristidis, Prog. Polym. Sci. [212] J.G. Sánchez, V.S. Balderrama, S.I. Garduño, E. Osorio, A. Viterisi, M. Estrada,
104 (2020). J. Ferré-Borrull, J. Pallarès, L.F. Marsal, RSC Adv. 8 (2018).
[167] F. Torres-Canas, J. Yuan, I. Ly, W. Neri, A. Colin, P. Poulin, Adv. Funct. Mater. 29 [213] S.H. Eom, H. Park, S.H. Mujawar, S.C. Yoon, S.S. Kim, S.I. Na, S.J. Kang, D. Khim,
(2019). D.Y. Kim, S.H. Lee, Org. Electron. 11 (2010) 1516–1522.
[168] J. Lim, H. Jung, C. Baek, G.T. Hwang, J. Ryu, D. Yoon, J. Yoo, K.I. Park, J.H. Kim, [214] S. Il Ahn, W.K. Kim, S.H. Ryu, K.J. Kim, S.E. Lee, S.H. Kim, J.C. Park, K.C. Choi,
Nano Energy 41 (2017) 337–343. Org. Electron. 13 (2012) 980–984.
[169] H. Xu, X. Hu, H. Yang, Y. Sun, C. Hu, Y. Huang, Adv. Energy Mater. 5 (2015), [215] M. Rai, L.H. Wong, L. Etgar, J. Phys. Chem. Lett. 11 (2020).
1401882. [216] F. Wang, J.H. Gosling, G.F. Trindade, G.A. Rance, O. Makarovsky, N.D. Cottam,
[170] Y. Lin, J. Chen, M.M. Tavakoli, Y. Gao, Y. Zhu, D. Zhang, M. Kam, Z. He, Z. Fan, Z. Kudrynskyi, A.G. Balanov, M.T. Greenaway, R.D. Wildman, R. Hague, C. Tuck,
Adv. Mater. 31 (2019), e1804285. T.M. Fromhold, L. Turyanska, Adv. Funct. Mater. (2021) 31.
[171] S. Wang, N. Liu, J. Tao, C. Yang, W. Liu, Y. Shi, Y. Wang, J. Su, L. Li, Y. Gao, [217] J. Shi, J. Jie, W. Deng, G. Luo, X. Fang, Y. Xiao, Y. Zhang, X. Zhang, X. Zhang,
J. Mater. Chem. A 3 (2015) 2407–2413. Adv. Mater. 34 (2022), 2200380.
[172] B. Li, N. Hu, Y. Su, Z. Yang, F. Shao, G. Li, C. Zhang, Y. Zhang, ACS Appl. Mater. [218] K. Liang, R. Wang, B. Huo, H. Ren, D. Li, Y. Wang, Y. Tang, Y. Chen, C. Song, F. Li,
Interfaces 11 (2019) 46044–46053. B. Ji, H. Wang, B. Zhu, ACS Nano 16 (2022) 8651–8661.
[173] J. Diao, J. Yuan, A. Ding, J. Zheng, Z. Lu, Macromol. Mater. Eng. (2018) 303. [219] Y.G. Kim, D. Lv, J. Huang, R.N. Bukke, H. Chen, J. Jang, Phys. Status Solidi 217
[174] K. Chi, Z. Zhang, J. Xi, Y. Huang, F. Xiao, S. Wang, Y. Liu, ACS Appl. Mater. (2020), 2000314.
Interfaces 6 (2014) 16312–16319. [220] K.J. Yoon, J.W. Han, D.I. Moon, M.L. Seol, M. Meyyappan, H.J. Kim, C.S. Hwang,
[175] N. Li, Y. Jiang, Y. Xiao, B. Meng, C. Xing, H. Zhang, Z. Peng, Nanoscale 11 (2019) Nanoscale Adv. 1 (2019) 2990–2998.
21522–21531. [221] E. Carlos, J. Deuermeier, R. Branquinho, C. Gaspar, R. Martins, A. Kiazadeh,
[176] X.F. Jin, C.R.L. Liu, L. Chen, Y. Zhang, X.J. Zhang, Y.M. Chen, J.J. Chen, Sensors E. Fortunato, J. Mater. Chem. C 9 (2021) 3911–3918.
Actuators A Phys. 316 (2020). [222] H. Hu, A. Scholz, C. Dolle, A. Zintler, A. Quintilla, Y. Liu, Y. Tang, B. Breitung, G.
[177] J. George, A. Abdelghani, P. Bahoumina, O. Tantot, D. Baillargeat, K. Frigui, C. Marques, Y.M. Eggeler, Adv. Funct. Mater. (2023), 2302290.
S. Bila, H. Hallil, C. Dejous, Sensors (Basel) (2019) 19. [223] S. Porro, C. Ricciardi, RSC Adv. 5 (2015) 68565–68570.
[178] A.S. Alshammari, M.R. Alenezi, K.T. Lai, S.R.P. Silva, Mater. Lett. 189 (2017) [224] J.U. Lind, T.A. Busbee, A.D. Valentine, F.S. Pasqualini, H. Yuan, M. Yadid, S.
299–302. J. Park, A. Kotikian, A.P. Nesmith, P.H. Campbell, J.J. Vlassak, J.A. Lewis, K.
[179] M.M. Kiaee, T. Maeder, J. Brugger, Adv. Mater. Technol. 6 (2020). K. Parker, Nat. Mater. 16 (2017) 303–308.
[180] C.J. Bright, E.C. Nallon, M.P. Polcha, V.P. Schnee, Anal. Chem. 87 (2015) [225] L. Zhou, X. Chen, W. Su, Z. Cui, W.Y. Lai, Adv. Mater. Interfaces 9 (2022),
12270–12275. 2102548.
[181] Y.Z.N. Htwe, I.N. Hidayah, M. Mariatti, J. Mater. Sci. Mater. Electron. 31 (2020) [226] T.K. Kang, Coatings 11 (2021) 51.
15361–15371. [227] E. Bihar, S. Wustoni, A.M. Pappa, K.N. Salama, D. Baran, S. Inal, NPJ Flex.
[182] G. Hassan, M.U. Khan, J. Bae, A. Shuja, Sci. Rep. 10 (2020) 18234. Electron. 2 (2018) 1–8.
[183] G. Hassan, J. Bae, A. Hassan, S. Ali, C.H. Lee, Y. Choi, Compos. Part A Appl. Sci. [228] L. Li, L. Pan, Z. Ma, K. Yan, W. Cheng, Y. Shi, G. Yu, Nano Lett. 18 (2018)
Manuf. 107 (2018) 519–528. 3322–3327.
[184] H. Minemawari, T. Yamada, H. Matsui, J. Tsutsumi, S. Haas, R. Chiba, R. Kumai, [229] V. Dua, S.P. Surwade, S. Ammu, S.R. Agnihotra, S. Jain, K.E. Roberts, S. Park, R.
T. Hasegawa, Nature 475 (2011) 364–367. S. Ruoff, S.K. Manohar, Angew. Chemie 122 (2010) 2200–2203.
[185] G. Mattana, A. Loi, M. Woytasik, M. Barbaro, V. Noël, B. Piro, Adv. Mater. [230] Y. Qin, H.J. Kwon, A. Subrahmanyam, M.M.R. Howlader, P.R. Selvaganapathy,
Technol. 2 (2017), 1700063. A. Adronov, M.J. Deen, Mater. Lett. 176 (2016) 68–70.
[186] X. Qiu, X. Gong, X. Zhang, W. Zheng, Coatings 12 (2022) 1893. [231] P. Lorwongtragool, E. Sowade, N. Watthanawisuth, R.R. Baumann,
[187] C. Wei, W. Su, J. Li, B. Xu, Q. Shan, Y. Wu, F. Zhang, M. Luo, H. Xiang, Z. Cui, T. Kerdcharoen, Sensors (Basel) 14 (2014) 19700–19712.
Adv. Mater. 34 (2022), 2107798. [232] M.J. Grotevent, C.U. Hail, S. Yakunin, D. Bachmann, M. Calame, D. Poulikakos,
[188] L. Liu, Y. Pei, S. Ma, X. Sun, T.J. Singler, Adv. Eng. Mater. 22 (2020), 1901351. M.V. Kovalenko, I. Shorubalko, Adv. Sci. 8 (2021), 2003360.
[189] C. Buga, J.C. Viana, Flex. Print. Electron. 7 (2022) 45004. [233] H.C. Wang, Y. Hong, Z. Chen, C. Lao, Y. Lu, Z. Yang, Y. Zhu, X. Liu, Nanoscale Res.
[190] H.M. Haverinen, R.A. Myllylä, G.E. Jabbour, Appl. Phys. Lett. 94 (2009). Lett. 15 (2020).
[191] J. Sun, Y. Li, G. Liu, S. Chen, Y. Zhang, C. Chen, F. Chu, Y. Song, ACS Appl. Mater. [234] G. Pace, A. Grimoldi, D. Natali, M. Sampietro, J.E. Coughlin, G.C. Bazan,
Interfaces 12 (2020) 22108–22114. M. Caironi, Adv. Mater. 26 (2014) 6773–6777.
[192] Nano Dimens. Https://Www.Nano-Di.Com/Ame-Dragonfly-Ldm (2021). [235] S. Ma, F. Ribeiro, K. Powell, J. Lutian, C. Møller, T. Large, J. Holbery, ACS Appl.
[193] T.T.T. Can, T.C. Nguyen, W.S. Choi, Sci. Rep. 9 (2019) 9180. Mater. Interfaces 7 (2015) 21628–21633.
[194] J. Im, Y. Liu, Q. Hu, G.F. Trindade, C. Parmenter, M. Fay, Y. He, D.J. Irvine, [236] G. Barrett, R. Omote, Inf. Disp. 26 (2010) 16–21 (1975).
C. Tuck, R.D. Wildman, Adv. Funct. Mater. (2023), 2211920. [237] L.M. Faller, W. Granig, M. Krivec, A. Abram, H. Zangl, J. Micromech. Microeng.
[195] F. Mathies, E.J.W. List-Kratochvil, E.L. Unger, Energy Technol. 8 (2020). 28 (2018), 104002.
[196] D. Dodoo-Arhin, R.C.T. Howe, G. Hu, Y. Zhang, P. Hiralal, A. Bello, [238] L.M. Faller, M. Lenzhofer, C. Hirschl, M. Kraft, H. Zangl, Sensors 19 (2019) 443.
G. Amaratunga, T. Hasan, Carbon N. Y. 105 (2016) 33–41. [239] S. Yang, N. Lu, Sensors 13 (2013) 8577–8594.
[197] X. Pi, L. Zhang, D. Yang, J. Phys. Chem. C 116 (2012) 21240–21243. [240] D. Barmpakos, A. Segkos, C. Tsamis, G. Kaltsas, Proceedings 2 (2018) 977.
[198] M.A. Green, Y. Hishikawa, W. Warta, E.D. Dunlop, D.H. Levi, J. Hohl-Ebinger, A. [241] M.D. Dankoco, G.Y. Tesfay, E. Benevent, M. Bendahan, Mater. Sci. Eng. B 205
W.H. Ho-Baillie, Prog. Photovoltaics Res. Appl. (2017) 25. (2016) 1–5.
[199] F. Mathies, T. Abzieher, A. Hochstuhl, K. Glaser, A. Colsmann, U.W. Paetzold, [242] C. Bali, A. Brandlmaier, A. Ganster, O. Raab, J. Zapf, A. Hübler, Mater. Today
G. Hernandez-Sosa, U. Lemmer, A. Quintilla, J. Mater. Chem. A 4 (2016) Proc. 3 (2016) 739–745.
19207–19213. [243] T. Vuorinen, J. Niittynen, T. Kankkunen, T.M. Kraft, M. Mäntysalo, Sci. Rep. 6
(2016) 35289.

19
A. Bastola et al. Materials Today Electronics 6 (2023) 100058

[244] A. Borenstein, O. Hanna, R. Attias, S. Luski, T. Brousse, D. Aurbach, J. Mater. [264] Y. Fang, X. Wu, S. Lan, J. Zhong, D. Sun, H. Chen, T. Guo, ACS Appl. Mater.
Chem. A 5 (2017) 12653–12672. Interfaces 10 (2018) 30587–30595.
[245] G. Li, Z. Meng, J. Qian, C.L. Ho, S.P. Lau, W.Y. Wong, F. Yan, Mater. Today Energy [265] J.A. Lim, J.H. Kim, L. Qiu, W.H. Lee, H.S. Lee, D. Kwak, K. Cho, Adv. Funct.
12 (2019) 155–160. Mater. (2010) 20.
[246] M. Maximov, D. Kolchanov, Il. Mitrofanov, A. Vinogradov, Y. Koshtyal, [266] M.F. Farooqui, M.A. Karimi, K.N. Salama, A. Shamim, Adv. Mater. Technol. 2
A. Rymyantsev, A. Popovich, Proceedings 3 (2018) 7. (2017), 1700051.
[247] C.A. Milroy, S. Jang, T. Fujimori, A. Dodabalapur, A. Manthiram, Small 13 (2017) [267] J. Kwon, Y. Takeda, R. Shiwaku, S. Tokito, K. Cho, S. Jung, Nat. Commun. 10
1–11. (2019) 54.
[248] S. Lawes, Q. Sun, A. Lushington, B. Xiao, Y. Liu, X. Sun, Nano Energy 36 (2017) [268] J. Kwon, Y. Takeda, K. Fukuda, K. Cho, S. Tokito, S. Jung, ACS Nano 10 (2016)
313–321. 10324–10330.
[249] P.E. Delannoy, B. Riou, T. Brousse, J.Le Bideau, D. Guyomard, B. Lestriez, [269] J. Kwon, Y. Takeda, K. Fukuda, K. Cho, S. Tokito, S. Jung, Adv. Electron. Mater. 2
J. Power Sources 287 (2015) 261–268. (2016), 1600046.
[250] J. Hu, Y. Jiang, S. Cui, Y. Duan, T. Liu, H. Guo, L. Lin, Y. Lin, J. Zheng, K. Amine, [270] K. Fukuda, Y. Takeda, Y. Yoshimura, R. Shiwaku, L.T. Tran, T. Sekine,
F. Pan, Adv. Energy Mater. 6 (2016), 1600856. M. Mizukami, D. Kumaki, S. Tokito, Nat. Commun. 5 (2014) 4147.
[251] F. Zhang, M. Wei, V.V. Viswanathan, B. Swart, Y. Shao, G. Wu, C. Zhou, Nano [271] J. Fang, W. Deng, X. Ma, J. Huang, W. Wu, IEEE Electron Device Lett. 38 (2016)
Energy 40 (2017) 418–431. 183–186.
[252] C.C. Ho, K. Murata, D.A. Steingart, J.W. Evans, P.K. Wright, J. Micromech. [272] K. Fukuda, T. Someya, Adv. Mater. 29 (2017), 1602736.
Microeng. 19 (2009), 094013. [273] W. Tang, Y. Huang, L. Han, R. Liu, Y. Su, X. Guo, F. Yan, J. Mater. Chem. C 7
[253] P.E. Delannoy, B. Riou, B. Lestriez, D. Guyomard, T. Brousse, J.Le Bideau, (2019) 790–808.
J. Power Sources 274 (2015) 1085–1090. [274] H. Cho, Y. Lee, B. Lee, J. Byun, S. Chung, Y. Hong, J. Inf. Disp. (2019) 0316.
[254] Elephantech Inc, Https://Www.Elephantech.Co.Jp/En/(2021). [275] T. Zhang, E. Asher, J. Yang, Adv. Mater. Technol. 3 (2018), 1700346.
[255] PV Nano Cell Ltd, Https://Www.Pvnanocell.Com/(2021). [276] M. Kang, K.T. Kang, Int. J. Precis. Eng. Manuf. Green Technol. 5 (2018) 421–426.
[256] BotFactory, Https://Www.Botfactory.Co/Page/Botfactory-Sv2-Pcb-Printer [277] Constantine A. Balanis, Antenna Theory: Analysis and Design, 4th Edn., John
(2021). Wiley & Sons, 2016.
[257] Nano Dimens. Https://Www.Nano-Di.Com/Ame-Materials (2021). [278] A. Alex-Amor, Á. Palomares-Caballero, J. Moreno-Núñez, A. Tamayo-Domínguez,
[258] J.S. Park, H.J. Choi, G.D. Han, J. Koo, E.H. Kang, D.H. Kim, K. Bae, J.H. Shim, C. García-García, J.M. Fernández-González, Microw. Opt. Technol. Lett. 63
J. Power Sources 482 (2021), 229043. (2021) 1719–1726.
[259] M. Kim, D.H. Kim, G.D. Han, H.J. Choi, H.R. Choi, J.H. Shim, J. Alloys Compd. [279] M.A. Monne, P.M. Grubb, H. Stern, H. Subbaraman, R.T. Chen, M.Y. Chen,
843 (2020), 155806. Micromachines 11 (2020) 1–12.
[260] L. Hakola, A. Parra Puerto, A. Vaari, T. Maaninen, A. Kucernak, S. Viik, [280] What Is PolyJet Technol. 3D Printing? | Strat. Https://Www.Stratasys.Com
M. Smolander, Flex. Print. Electron. 5 (2020), 025002. /Polyjet-Technology (2021).
[261] E. Sowade, M. Polomoshnov, A. Willert, R.R. Baumann, Adv. Eng. Mater. 21 [281] M.F. Farooqui, A. Shamim, IEEE Antennas Wirel. Propag. Lett. 16 (2017)
(2019), 1900568. 800–803.
[262] K. Kowsari, S. Akbari, D. Wang, N.X. Fang, Q. Ge, 3D Print, Addit. Manuf. 5 [282] J. Kimionis, M. Isakov, B.S. Koh, A. Georgiadis, M.M. Tentzeris, IEEE Trans.
(2018) 185–193. Microw. Theory Tech. 63 (2015) 4521–4532.
[263] A. Scholz, L. Zimmermann, U. Gengenbach, L. Koker, Z. Chen, H. Hahn, A. Sikora, [283] T. Tilford, S. Stoyanov, J. Braun, J.C. Janhsen, M.K. Patel, C. Bailey, IEEE Trans.
M.B. Tahoori, J. Aghassi-Hagmann, Nat. Commun. 11 (2020). Compon. Packag. Manuf. Technol. 11 (2021) 351–362.

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