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RESEARCH ARTICLE

www.advsensorres.com

A Paper-Based Triboelectric Touch Interface: Toward Fully


Green and Recyclable Internet of Things
Jesper Edberg,* Ulrika Boda, Mohammad Yusuf Mulla, Robert Brooke, Sandra Pantzare,
Jan Strandberg, Andreas Fall, Konstantin Economou, Valerio Beni, and Astrid Armgarth

the origin and processing of materials,


The transition to a sustainable society is driving the development of green production of electronics components,
electronic solutions designed to have a minimal environmental impact. One usage, and disposal/destruction. With
promising route to achieve this goal is to construct electronics from biobased the trend of the internet-of-things (IoT)
materials like cellulose, which is carbon neutral, non-toxic, and recyclable. steadily growing, electronic devices are
being integrated into every aspect of our
This is especially true for internet-of-things devices, which are rapidly growing everyday lives.[4–6] As the number of con-
in number and are becoming embedded in every aspect of our lives. Here, nected devices increases, so does the
paper-based sensor circuits are demonstrated, which use triboelectric problem of electronic waste.[7,8] For this
pressure sensors to help elderly people communicate with the digital world reason, there is a drive to develop green
using an interface in the form of an electronic “book”, which is more intuitive IoT electronics to minimize this grow-
ing problem. One way to tackle the prob-
to them. The sensors are manufactured by screen printing onto flexible paper
lem is to build electronics based on bio-
substrates, using in-house developed cellulose-based inks with mass sources such as wood.[9–11] This re-
non-hazardous solvents. The triboelectric sensor signal, generated by the newable source of the material is car-
contact between a finger and chemically modified cellulose, can reach several bon neutral as opposed to synthetic ma-
volts, which can be registered by a portable microcontroller card and terials based on petroleum such as plas-
transmitted by Bluetooth to any device with an internet connection. Apart tics, and it has the added advantage of
being biodegradable which means that
from the microcontroller (which can be easily removed), the whole system can it will not contribute to landfills and
be recycled at the end of life. ocean microplastics, which never fully
breaks down and can bioaccumulate and
biomagnify.[12] Besides being used as
1. Introduction a structural material, wood derivatives
such as cellulose and lignin can also have an electronic or
Green electronics is the collective term for technologies where electrochemical function; properties which have been used
the full environmental impact is considered and where nega- to manufacture bio-based electronics such as batteries,[13,14]
tive effects have been minimized or eradicated.[1–3] This includes supercapacitors,[15,16] sensors,[17] and energy-harvesters.[18] This

J. Edberg, U. Boda, M. Y. Mulla, R. Brooke, S. Pantzare, J. Strandberg, U. Boda


V. Beni, A. Armgarth Linköping University
RISE Research Institutes of Sweden Department of Science and Technology (ITN)
Digital Systems Laboratory of Organic Electronics
Printed-, Bio- and Organic Electronics SE-601 74 Norrköping, Sweden
Bredgatan 35, SE-602 21 Norrköping, Sweden A. Fall
E-mail: jesper.edberg@ri.se RISE Research Institutes of Sweden
J. Edberg, U. Boda, M. Y. Mulla, R. Brooke, S. Pantzare, A. Fall, V. Beni Bioeconomy & Health, Smart Materials
Digital Cellulose Center Drottning Kristinas väg 61, SE-114 28 Stockholm, Sweden
Bredgatan 35, SE-602 21 Norrköping, Sweden K. Economou
Linköping University
Department of Culture and Society
Division of Culture
The ORCID identification number(s) for the author(s) of this article
Society
can be found under https://doi.org/10.1002/adsr.202200015
Design and Media (KSFM)
© 2022 The Authors. Advanced Sensor Research published by SE-601 74 Norrköping, Sweden
Wiley-VCH GmbH. This is an open access article under the terms of the
Creative Commons Attribution License, which permits use, distribution
and reproduction in any medium, provided the original work is properly
cited.
DOI: 10.1002/adsr.202200015

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new research field goes under different names including paper the MediaBook, is designed to be used as a more intuitive and
electronics or digital cellulose. user-friendly interface to other digital medias.
Besides the materials being used, the method of producing
electronics is also important to be considered “green”. This in- 2. Results and Discussion
cludes the energy consumption and chemicals used for process-
ing. Printed electronics (PE) is the method of producing elec- 2.1. Sensor Structure and Signal-To-Noise Ratio
tronic components using traditional or novel printing methods
with the use of functional inks.[19–22] PE has several advantages Although many types of touch sensors exist (i.e., resistive and
over classical electronics manufacturing such as low processing capacities), triboelectric sensors have the advantage that they are
temperatures (resulting in lower energy consumption) and less self-powered, that is they produce their own signal (voltage) upon
hazardous chemicals (such as strong acids used for metal etch- pressure stimuli.[26] This is different from for example resistive
ing). Therefore, PE can be considered “greener” as compared to or capacitive sensors which require that a continuous stimulus
classical electronics. (a current or a voltage) is delivered from the measurement appa-
One more environmental aspect of IoT is the energy used to ratus and the sensor response is continuously recorded. Subse-
power distributed devices.[23,24] Since it is not practical to use ca- quently, triboelectric sensing has the advantage that the readout
bles connected to the power grid, most IoT devices rely on bat- electronics can be in a low-power “deep sleep state” until it is
teries for power. However, batteries have a limited lifetime, and awakened by an interrupt generated after touch. In this work,
replacing them is often not an option if the devices are placed in a triboelectric touch-sensor using wood-based materials in the
remote locations, embedded into larger systems, or just because sensing layer, the electrical conductors, as well as the substrate,
of the sheer number of the devices. For this reason, much re- was developed and produced using widely employed mass fabri-
search is focused on developing energy-autonomous systems that cation technique of screen printing (Figure 1a).
can harvest power from their surroundings.[24,25] These power The sensors reported herein are based on single electrode
sources can be light, heat, movement, or RF radiation, to name mode (illustrated in Figure 1b) TENG.[34] This consists of a con-
a few. One of the more recent energy harvesting technologies is ductive layer called the charge collector (in this work the carbon
triboelectric nanogenerators (TENG) which can convert mechan- electrodes), and a dielectric layer called the electrification layer,
ical energy into electrical energy.[26,27] These devices share many friction layer, or simply triboelectric layer (in this work the nitro-
characteristics with piezoelectric energy harvesters, but they can cellulose coating).[35,36] Triboelectric signals are generated when
be constructed from a wider range of materials and can generally a free-standing electrification layer (in this work human skin)
harvest more power than by using the piezoelectric effect. TENG comes into contact with the device electrification layer, inducing
has been explored for a large number of applications, including in this way a transfer of surface charges between the two mate-
sensing and human-machine interactions.[28] rials. When the layers are separated, the surface charges persist,
In this work, we have developed flexible, printed, and paper- and the sign (positive or negative) of the accumulated charge will
based triboelectric touch/pressure sensors working as a human- depend on the relative position of the two materials (cellulose and
machine interface for IoT applications. TENG devices have skin) in the so-called triboelectric series (Figure 1c) with the mate-
shown great promise as an electronic interface for body param- rials higher in the series giving, upon contact, electrons to those
eters such as pressure upon touch,[29,30] eye movement,[31] or lower in the series.[37] Finally, since the charge collector is con-
as hearing aids.[32] Typically, printed electronics use plastic sub- nected to the electrical ground, the accumulated charges will in-
strates since they have a flat surface and are less sensitive to am- duce a current (to balance the charges at the electrification layer),
bient conditions such as humidity. However, since plastic is cur- which becomes the sensor signal.
rently one of our biggest waste problems, the transition to more One issue with the use of cellulose to detect, via triboelectric
sustainable materials is crucial.[33] To this end, we produced the devices, the touch of a finger is that a low voltage is typically gen-
sensors and circuits on paper substrates, which can be made to erated since cellulose, wood, paper, and other bio-based materi-
be biodegradable (as to not contribute to bioaccumulation of mi- als are positioned close to the human body (i.e., skin) in the tri-
croparticles) and CO2 neutral. Besides the substrate, also the tri- boelectric series.[38,39] Subsequently, in this work cellulose was
boelectric material which generates the sensor signal was based replaced with nitrocellulose (NC), which is more electronegative
on cellulose, and a printable cellulose ink was developed. We used and hence has a position lower down in the triboelectric series
printed carbon for the conducting lines and charge collectors to (Figure 1c).[40,41] This separation is enough to generate a voltage
build metal-free electronics. We explored both commercial car- large enough to be useful for sensing applications while being
bon inks as well as an in-house developed carbon ink that uses not too large to damage the low-power electronics employed for
nanocellulose as the binder. Also, we used only environmentally readout.
friendly solvents for the developed inks to further minimize the Figure 1d shows the schematics of two different sensor cir-
environmental impact, but also to lower the hazard risks for hu- cuits, one with circular sensor electrodes and one with an inter-
mans during production. The sensors were further demonstrated digitated structure, that were designed and evaluated. The circu-
in a portable electronics application in the form of an electronic lar design most closely resembles that of the generalized struc-
book for elderly people, with content produced in collaboration ture shown in Figure 2a, as it consists of just a single charge
with the seniors themselves or with relatives, allowing for the collector and electrification layer. The problem with this design
personalization of both the content and the contexts of use. Since is that for portable electronics applications, there is not always
many elderly people have a difficult time using modern digital de- an obvious ground point to connect to. This can lead to a large
vices such as smartphones or tablets, this book, which is called amount of electronic noise, which can make it difficult for the

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Figure 1. a) Schematic of the sensor concept. b) Schematic of TENG single-electrode mode with material cross sections. c) Triboelectric series. d)
Schematics of two different sensor circuit patterns. e,f) Voltage response to finger tapping TENG sensor, with two different sensor structures. g) Sensor
noise level for the two designs, with/without NC coating and with/without a finger statically pushing on the sensor (open vs. holding).

readout electronics to detect a clear signal. To investigate the direction), even though they have very different electrode areas
effect of the ground point on the noise level, a second design (3.14 cm2 for circular and 1.24 cm2 for IDE). This voltage level is
based on two electrodes (sensing electrode and ground electrode) more than enough for reading out the signal, but not too large,
finger-like structure (interdigitated electrodes, IDEs) was created which could damage the readout electronics in portable applica-
(Figure 1a). In early measurements with the circular design, it be- tions (see section “Portable electronics and wireless communica-
came apparent that less noise was generated when touching the tion”).
sensor if the user was also touching a metal wire connecting to The sensor in this work generates short voltage spikes upon
the electrical ground of the measurement equipment. However, contact, so, it is important that no signals are generated when no
holding a ground cable is not practically useful in any real-life ap- finger is touching or when a finger is touching statically (pushing
plication, so, the idea behind the interdigitated structure was to for a long time rather than tapping with the finger) since this
mimic this configuration while only touching the electrode area. would make the application trigger at the wrong time. For this
When a finger comes in contact with the IDE sensor, it will bridge reason, an investigation into the sensitivity of the printed circuits
the gap between the electrodes, thus creating a similar setup to to electronic noise was conducted. Figure 1g shows the electronic
holding the ground cable and thereby generating a more stable noise level (background noise) for the two sensor designs (inter-
electrical signal. The “fingers” in the sensor electrodes were made digitated and circular) with or without NC coating on top, and
wider (1.26 mm, to maximize contact area) than the ground “fin- with or without a finger pushing down statically on the sensor. A
gers” and were coated with nitrocellulose, while the ground elec- similar noise level (≈75–100 mV) was observed for both sensor
trodes (0.66 mm) were uncoated, that is, only carbon. The over- designs, with and without NC coating, when no finger was touch-
all circuit design was made to fit in the MediaBook (see the sec- ing. For the IDE design, the noise would decrease to <50 mV
tion “Portable electronics and wireless communication” as well when pushing with a finger. This is because the body becomes
as Supporting Information), where each sensor is connected to a grounded through contact with the bare carbon electrode fingers,
contact pad by a conductor line. The contact pads are further used which reduces noise. In contrast, the circular design had a large
to connect to the electronic readout system. Figure 1e,f shows the increase in noise level upon contact with a finger, reaching values
generated voltage from the two different sensor structures when of 400–500 mV. While the voltage generated by the sensors in
tapping with a finger. Interestingly, the signal strength from the Figure 1e,f shows large variations due to the irreproducible pres-
two sensor structures is very similar (≈2 V in the positive voltage sure when tapping with a finger, the values are still comparable

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Figure 2. a) Molecular structure of the NC ink components. b) Photographs of NC inks using propylene glycol (left) and dipropylene glycol (right) as
solvents. c) Rheology data of NC ink with different solid content. d) Photograph of a printed circuit on a paper substrate. e) Sheet resistance data for the
different carbon inks, and carbon coated with different number of layers of NC. f) Resistance of printed carbon conductor lines during bending tests at
different bending radii, with “Rest” indicating the values between bending tests.

at ≈2 V peak voltage in the positive direction. Taking this value was needed. While NC can easily be dissolved in acetone, this is
as the “signal value”, the signal-to-noise ratio (Vsignal /Vnoise ) of not a suitable solvent for screen-printing due to its low boiling
the IDE design is ≈46 while for the circular design it was ≈4. point which can cause rapid evaporation, leading to drying of
This shows that a tenfold increase in signal-to-noise ratio can be the inks in the printing frames, causing clogging. Furthermore,
achieved using the IDE design rather than the “classical” single acetone can also damage the screen printing frames, and the
electrode design which is most often reported in literature. While produced volatiles are hazardous to humans. Instead, we looked
the signal level in Figure 1e is large enough to not be confused for a higher boiling point solvent with no hazards. Propylene
with any noise generated by the surroundings or by holding glycol (boiling point of 188,2 °C) and dipropylene glycol (boiling
the sensor, this might not be the case for a gentler tapping than point (230,5 °C) were investigated as they are both non-toxic.
what was used to record this dataset. Since the sensor signal When performing solvent exchange from acetone to propylene
is proportional to applied pressure (see section “Triboelectric glycol (see Experimental Section) the polymer sedimented at the
characterization”), the noise level sets the limit to how small bottom of the vial. However, when trying the even higher boiling
pressure can accurately be registered. The electronic noise data point dipropylene glycol, this time, a stable solution could be
in Figure 1g was derived from Figure S1 (Supporting Informa- obtained. Figure 2b shows photographs of inks prepared with
tion). A video of sensors generating voltage peaks on a portable propylene glycol (left) and dipropylene glycol (right). In the left
oscilloscope can be seen in Video S1 (Supporting Information). photograph, the white NC can be seen to sediment at the bottom
while no residues could be found in the perfectly transparent
dipropylene glycol mixture.
2.2. Ink Formulation and Printing The ink was prepared with different concentrations of NC (10,
20, 30, and 40 mg ml−1 ) and their rheological properties were
While NC has been used in the past in triboelectric characterized using a rheometer. In screen printing, the ink
applications,[18,40] to the best of our knowledge it has not should have the property that the viscosity decreases at applied
been used in a printed electronics manufacturing process. NC is shear force, so-called shear thinning.[42] This ensures that the
usually prepared by treating cellulose with a mixture of nitric and ink flows easily during printing but becomes more viscous after
sulfuric acid, as depicted in Figure 2a and has historically been printing which prevents it from spreading. Figure 2c shows
used in many products such as ping pong balls and celluloid the rheology graphs of viscosity vs. shear speed. The lowest ink
film. Since NC does not dissolve in water, an organic solvent concentration had a very low viscosity which did not change

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with increased shear speed. With increasing concentration, the not dissolve in water (Figure S3d, Supporting Information) but
desired shear thinning appears, and at 40 mg ml−1 , the ink was that the combination of wetting and rubbing was needed (Figure
viscous enough to easily handle while also printing well due to S3e,f, Supporting Information). Since this kind of washing step
the lowering of viscosity at higher shear speed. Even higher con- (wetting and mechanical force) is typical for paper recycling to
centrations resulted in inks that were too viscous to be printable remove inks and other additives (a process known as de-inking),
(no further characterization was done on these). The 40 mg ml−1 we believe that the technology is truly recyclable. Also, beyond
concentration was therefore used for the printing of the sensors. recyclability, paper made from only cellulose will naturally biode-
The printed circuits consisted of carbon conductors and charge grade if it ends up in landfills or in the sea.
collectors, an NC electrification layer, and a lacquer layer meant
to protect the carbon lines from scratches during the assembly of
the MediaBooks. The lacquer layer however turned out to not be 2.3. Triboelectric Characterization
necessary (although it was used for most prints) since the printed
carbon showed good adhesions to the paper. The frames used for While the sensors were demonstrated to work with direct con-
the printing can be seen in Figure S2 (Supporting Information). tact with skin (Figure 1), performing repeatable quantitative mea-
Figure 2d shows a photograph of a printed sensor circuit on a pa- surements require an automated setup. To this end, a measure-
per substrate. Since the NC remains transparent after printing, it ment setup with a linear actuator arm and an adjustable stage
cannot be seen easily by the naked eye. However, the presence of was constructed (see Experimental Section and Figure S4, Sup-
NC was confirmed by measuring the electrical surface resistance. porting Information). The frequency of the linear actuator of the
Three different types of carbon inks were used in the study: two arm could be controlled and acted as a replacement for the finger.
commercial inks and one in-house prepared. The in-house pre- The triboelectric sensors were placed on the base plate attached
pared carbon ink (which we call CNF-C in the manuscript) is wa- to a movable stage which position could be controlled with a pre-
ter based and uses cellulose nanofibrils (CNF) as the ink binder. cision using a micromanipulator screw. By adjusting the position
In contrast, commercial carbon inks are solvent based and use of the plane, the impact force of the arm on the sensor could be
synthetic binders. Figure 2e shows the sheet resistance of the dif- controlled. The relative impact force was measured using a com-
ferent carbon inks used with a different number of NC layers on mercial piezoelectric sensor placed behind the reusable adhesive
top. One or two layers of NC show an unchanged sheet resistance, over which samples were mounted. This piezo sensor however
however, at three layers the resistance reached values outside the does not provide absolute force values but allowed us to adjust
measurement range (>10 MΩ sq−1 .) indicating a full coverage the position of the base plate such that the relative impact forces
with no pinholes. The three carbon inks show a large variation were consistent in all measurements. A piece of natural leather
in resistance, with the in-house prepared ink having the highest was attached to the actuator arm to mimic the contact between
resistance. The commercial 7102 carbon ink was used for its com- the sensor and a finger.
paratively low sheet resistance to see if this would influence the Sensors with different number of layers of printed NC were
sensor performance, and a commercial stretchable carbon was produced and the generated peak-to-peak voltage (Vpp ) was
used to see if it would perform better during the bending of the recorded. The results in Figure 3a shows that even one layer of
substrates. Since the printed sheets need to be bent during the as- NC is enough to produce a signal. However, the generated volt-
sembly into the MediaBook device, bending tests were performed age increases with the number of layers up to 3 layers and then
on conductor lines using the three carbon inks. The results can stabilizes. This indicates that the first and second layers do not
be seen in Figure 2f where the lines were bent around rods with cover completely the underlaying carbon electrode, which is in
different bending radii. As can be seen from the graph, the re- agreement with the sheet resistance data from Figure 2e. If there
sistance of the conductor lines did not change to any significant are pinholes present in the NC coating, some charges that accu-
degree for any of the carbon prints. However, it should be noted mulate on the surface during TENG operation can be discharged
that the bent area is only a small part of the total length of the through the holes to the carbon charge collectors. This loss in
line. surface charge will also results in a lower generated voltage. It is
The paper substrates used for most of the investigations in therefore important to have a full coverage of the electrification
this work are not 100% cellulose-based (which is the case for layer to achieve optimum performance.
most papers which usually contain different fillers) but contained The voltage response of circular and interdigitated sensors was
wet-strength polymers. This paper was used since it had an ideal also studied, and these can be seen in Figure 3b,c, respectively.
thickness, mechanical properties, and heat resistance to fit into Both sensors’ structures show similar voltage magnitude and
the final application (see the section “Portable electronics and an asymmetry in the positive and negative voltage peaks (also
wireless communication”). However, due to the unknown origin observed in Figure 1e,f using a finger). Such asymmetry is of-
of the additive, the recyclability of the paper sheets becomes ques- ten observed in TENGs and has been explained by an adhesion-
tionable. In order to show that the sensor sheets can be made induced impulsive separation.[43] Figure 3d shows the mean volt-
truly recyclable, we further manufactured the circuits on paper age generated by the two types of sensor designs and using two
containing 100% cellulose (see Figure S3, Supporting Informa- types of carbon ink with a large difference in sheet resistance
tion). We showed that these sensors performed as well as the (see Figure 2f). For the interdigitated sensors, no difference in
ones printed on the wet-strength paper (Figure S3a,b, Supporting voltage level could be seen by using carbon inks with higher or
Information) and demonstrated that the carbon conductors and lower resistance. This shows that the in-house prepared aque-
NC can be washed away by first wetting the sheets followed by ous cellulose-based ink can be used without loss in performance,
mechanical force (rubbing). It should be noted that the inks did and so the commercial ink using synthetic binders and the or-

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Figure 3. a) Mean Vpp of interdigitated sensor with different numbers of printed NC layers. b) Voltage response of circular sensor. c) Voltage response
of interdigitated sensor. d) Mean Vpp for different sensor structures and different carbon inks. e) Vpp of a sensor with different load resistance. f) Vpp of
a sensor with different relative pressure, measured by the response of a piezo sensor.

ganic solvent was not used in further measurements or in the portant design information when choosing the impedance in the
final application. While the circular designs show larger voltage portable readout electronics for the MediaBook. Figure S6 (Sup-
values, the large error bars in the circular sensor using CNF-C porting Information) shows the calculated peak power values for
carbon make it difficult to draw any conclusions. It does however the same data as in Figure 3e.
appear like the circular design with its larger surface area could Finally, we investigated if the voltage signal was dependent on
have an advantage when it comes to the produced voltage. How- the impact force of the actuator. This is the case for piezoelectric
ever, it should be noted that the values shown in the figure are the sensors which work by compressing the material, but not neces-
peak-to-peak voltage values. Figure S5 (Supporting Information) sarily for TENG devices which work on a different physical prin-
shows that there is a difference in the ratio between the positive ciple. Figure 3f shows Vpp versus the voltage of the piezoelectric
and negative voltage peaks for the two sensor designs, with the in- pressure sensors placed behind the triboelectric sensor. We can
terdigitated being more asymmetrical. This means that the volt- see that the two voltage signals have a linear dependence. Since
age peak in only the positive direction is more similar between the piezoelectric sensor generates a voltage that is linear to the
the two designs. Since this is the level, which is measured in applied pressure, this shows that also the TENG device has a lin-
the MediaBook application, there is little advantage in using the ear response to pressure and can be used for such applications.
circular design. Instead, the interdigitated design with its high One important question is the lifetime of the touch sensors.
signal-to-noise ratio was deemed to be the more advantageous Since the triboelectric effect is based on friction, any such system
design. will eventually degrade. But the rate of degradation will largely
The voltage that can be measured upon impact depends on depend on the choice of materials, architecture, mode of oper-
the load over which it is measured. Typically for TENG, a load be- ation, as well as the applied force. Since paper is generally not
tween 1–100 MΩ is required to achieve maximum voltage and a very durable material compared to synthetic materials such as
power.[44] Figure 3e shows the Vpp of an interdigitated sensor plastics, this question of durability becomes even more impor-
which was measured while varying the load resistance. The ef- tant. Figure S7 (Supporting Information) shows the voltage re-
fective load is the parallel connection of the external load and sponse of a sensor during 50 000 cycles in the actuator setup.
the internal load of the measurement equipment (10 MΩ), which The frequency was set to 2 Hz to mimic the tapping speed of a
limited the values to 5 MΩ in our setup. We can see that the volt- finger, and the voltage response was periodically measured (ini-
age increases more sharply for the smaller values of the load and tial values, after 20 000, 40 000, and 50 000 cycles). Surprisingly,
then decreases to finally give a linear increase. This is likely due no degradation was visible from the voltage signal during the first
to the limited input impedance of the measurement equipment 40 000 cycles, and after the full 50 000 cycles, there was even an in-
and indicates that the voltage can be higher if the impedance of crease in the signal strength. One possible explanation is that the
the measurement equipment is increased. This also gives im- friction causes a roughening of the nitrocellulose surface which

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Figure 4. Scanning electron microscopy images of different printed carbon layers (a–f) and different number of NC layers on carbon (g–j).

increases the effective contact area. For further details on how circuits with voltage dividers will be needed to circumvent this
the frequency of operation affects the triboelectric signal, see Fig- issue.
ure S8 (Supporting Information) and the associated discussion in
Supporting information.
The performance of the sensors in this work was compared 2.4. Scanning Electron Microscopy
with recent similar publications on triboelectric touch sensors.
Table S1 (Supporting Information) lists the materials (triboelec- The microscopic structure of the three types of printed carbon
tric material, charge collector, and substrate) and generated volt- on paper, as well as NC coatings on carbon was investigated us-
age of 8 previous publications. The literature survey was limited ing scanning electron microscopy (SEM). Figure 4a–f shows the
to only publications where the single electrode mode was used structure of the two commercial screen-printing carbons (7102
and where the main theme was TENG as a touch sensor. Among and CI-2051), as well as the in-house, made carbon ink (CNF-C)
the reviewed publications, there was none that used biobased ma- which used cellulose nanofibrils as the binder. At low magnifi-
terials in any of the layers. Typically, synthetic materials like poly- cation (Figure 4a–c), it is clear that the CNF-C carbon is thin-
dimethylsiloxane and poly(ethylene terephthalate) were used for ner than the commercial carbons as the underlying fibers of the
the triboelectric layer and substrate respectively, and metals or paper substrate can be seen. However, although the films were
metal oxides were used for the charge collectors. The generated thin, the higher magnification image (Figure 4f) shows that the
voltage of the prior art sensors was in the same order of mag- coating is continuous at microscopic scale and without apparent
nitude as this work, with the exception of two references where pinholes, like the commercial inks (Figure 4d,e). Even though
up to 100 V could be generated. It should however be noted that the CNF-C carbon conductors were thin, and the resistance of
for sensor applications, such high voltages will be problematic, the obtained conductor lines was considerably higher (Figure 2),
as they can damage the readout electronics, and more complex the continuous coating ensures good triboelectric performance

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Figure 5. a) Sensor response read by a microcontroller with two sensor channels connected and transmitted to the computer by Bluetooth. The sensors
were pressed with the backside of a finger to eliminate the effect of finger moisture which gave varying results. b) Sensor response while tapping or
holding a sensor with constant pressure. c) Schematic of the MediaBook operation flow. d) Photographs of the MediaBook front cover, e) inside the book,
f) and the embedded MCU card. g,h) Photographs of MediaBook in operation as pushing the buttons activated and changes a photograph slideshow
in the computer (see Video S2, Supporting Information).

as shown in Figure 3. Figure 3d shows that there is little differ- tration (40 mg mL−1 ), it is unlikely that the thickness should be
ence in the magnitude of the triboelectric signal for the differ- undetectable. It is more likely that the carbon electrode is porous
ent carbon ink types, and Figure S5 (Supporting Information) enough that it absorbs the ink during printing, instead of only
shows that there is no difference in the peak ratio between the ending up on the top. This explains why there is not complete
carbon with the lowest and highest resistance. The combined re- coverage after just a single print. With the increasing number of
sults show that the cellulose-based carbon performs as good as prints, the pores get filled in by the NC and eventually cover all
commercial inks in the triboelectric sensors with an added ad- the carbon at the top surface after 3–5 printed layers.
vantage of not containing any synthetic binders and using envi-
ronmentally friendly solvents.
SEM of the NC-coated structures (Figure 4g–j) indicates that 2.5. Portable Electronics and Wireless Communication
nitrocellulose makes the surface more insulating with the in-
creasing number of coated layers, based on the diminishing pres- In the TENG characterization so far, the triboelectric response
ence of granular brighter conducting carbon particles visible, was measured using an oscilloscope, which is an advanced,
while the surface appears increasingly smooth due to the non- costly, and bulky equipment. To demonstrate the feasibility of
conductive material on top. At two layers of nitrocellulose in Fig- using the paper-sensors in real-life IoT applications, we here
ure 4h, several dark pinholes can be seen. At 3 layers only a single show the integration with a low-cost and low-power portable
pinhole can be seen and at 4 layers no pinholes were detected. electronics card equipped with wireless BLE (Bluetooth Low
This explains the results from Figure 2e and Figure 3a which Energy) communication. Figure 5g shows a photograph of the
showed an increase in sheet resistance and voltage respectively in-house developed printed circuit board (PCB) with a microcon-
with the number of layers up to 3–4 layers after which little dif- troller used for collecting data from the sensors. Figure 5a shows
ference was detected. Figure S9 (Supporting Information) shows the data from the microcontroller when two sensor channels
the thickness of the printed coatings of carbon and nitrocellulose of the interdigitated structure were connected. The two sensors
(combined thickness) with respect to the number of printed NC (TENG1 and TENG2) were positioned close to each other as
layers. The graph shows that the carbon layer is ≈4 μm thick, but indicated in the photograph in Figure S10 (Supporting Informa-
that there appears to be no increase in the thickness as the nitro- tion). When tapping TENG1 with a finger, clear voltage signals
cellulose is added. Since the nitrocellulose ink has a high concen- were registered while only a small crosstalk could be detected in

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the neighboring TENG2 channel, and vice versa. While the two communication. A video of this can be found in Supporting In-
sensors were located with a few centimeters distance from each formation (Video S2, Supporting Information).
other, the corresponding conductor lines were only millime-
ters apart. Even so, the electronic crosstalk can be considered
negligible, which is of great importance when using multiple 3. Conclusion
sensors in a circuit. No additional amplifying electronics was
needed to capture the signals which were registered directly by In this work, we have developed and manufactured a bio-
the analog inputs of the microcontroller Figure 5b further shows based and metal-free touch-sensor circuits working as a human-
the signals from TENG1 when tapping compared to applying a machine interface. Functional inks, containing active materi-
constant pressure using a finger. Moreover, as described in the als employing environmentally friendly solvents, were developed
previous section, the TENG voltage was just enough to trigger and the touch sensor circuits were patterned on flexible pa-
signals to be measured by (analog to digital converter) ADC of per substrates using screen printing. The carbon-based electrical
the microcontroller, while not too high which could damage the conductor circuits showed a negligible difference in resistance
microcontroller. Only a small capacitive electronic noise could be when bending down to 2 mm radius. Strong triboelectric signals
registered during the constant pressure, showing that the good of several volts could be generated by the sensors when coming
signal-to-noise level of the interdigitated sensors persist also for in contact with skin, and the novel design enhanced the signal-
the portable electronics readout. It can be noted that the signal in to-noise ratio by an order of magnitude. Beyond touch sensitivity,
Figure 5a is slightly lower than that shown for finger tapping in the sensors also demonstrated a linear response to applied pres-
Figure 1f. This difference is likely due either to the difference in sure, which could widen the possible application areas of such
input impedance between the oscilloscope and the portable elec- paper-based TENG sensors. We further combined the sensors
tronics or by a difference in finger moisture at the two measure- into a portable low-power electronic sensor readout platform that
ment times. However, the most important property of the sensor could record signals and transfer information by wireless Blue-
signals is that they can be clearly distinguished from any noise or tooth communication. This setup was further integrated into an
crosstalk. electronic paper-based “book” which will be used as a more in-
Although the developed sensors can have a wide range of uses, tuitive human-machine interface for elderly people that struggle
the printed circuits were designed to be used for a particular IoT with modern technology. Besides the easily detachable readout
application, namely as the human-machine interface in an elec- PCB, we showed that the whole electronic system can be dis-
tronic album, shaped and designed like a picture book with card- posed as paper trash at end of life. Overall, we have shown the
board pages. This “MediaBook” is meant to be used as an intu- feasibility of manufacturing fully bio-based and environmentally
itive interface to electronic media content for elderly people. The friendly green electronics to be used in IoT applications. This is
rationale behind the idea is that elderly people sometimes have a necessary step to reduce the growing threat of electronic waste
difficulties using electronic interfaces like the touch screens on and to become more sustainable with respect to materials and
smartphones and tablets which limits their possibilities of uti- the manufacturing of electronics in general.
lizing modern technology. This is both a problem of hand/eye
coordination, but also because capacitive touch displays are not 4. Experimental Section
optimized for the dryer skin of elderly people, sometimes leading
Ink Preparation: The carbon ink using CNF binder (CNF-C) was pre-
to a poor sensitivity. There can also be a mental barrier to over-
pared by adding carbon black (CB) powder to premade CNF suspensions
come with elderly people using technology that seems foreign to then mixed by high-pressure homogenization. Carboxymethylated CNF
them.[45] For this reason, the MediaBook was developed to bridge with a degree of substitution of 0.1, homogenized 1 pass at 1700 bar, was
the gap and let people of all ages get the benefits that modern used. This 1 wt.% CNF gel was diluted to 0.4 wt.% by adding deionized
technology and media can offer. The book, seen in one version in water and gently stirring it overnight. CB powder was added to 1 L of the
Figure 5e,f, has touch buttons on each page along with text and diluted gel to a ratio of 15:1 CB to the dry mass of CNF and homogenized,
2 passes at 400 bar. This provided a total solid content of 6.4 wt.%. The ink
photographs. As shown in the flow diagram of Figure 5c, pushing
preparation method and composition were previously reported in greater
a button on a page will generate a voltage signal which is regis- detail.[47]
tered by the microcontroller on the PCB embedded in the book. The nitrocellulose ink was prepared by first dissolving nitrocellulose
The card further sends a signal to an external media by a wireless blotting paper (GE Healthcare Life Science, No. 10600002) into acetone
Bluetooth connection (see Figure S11, Supporting Information) at a concentration of 80 mg ml−1 while stirring with a magnet bar. Propy-
for a schematic of the microcontroller card). Figure S12 (Sup- lene glycol or dipropylene glycol was added to the mixture and stirred un-
porting Information) shows the integration of the printed circuits til homogenous. The acetone was subsequently evaporated by heating at
70 °C while stirring. The final concentration of the ink was 10, 20, 30, or
into the MediaBook and the connection to the readout electron- 40 mg ml−1 depending on the added amount of propylene/dipropylene
ics. The media platform can for example be a smartphone or a glycol.
tablet (or any other device with an internet connection), which Rheological profiles were recorded with an MCR 102 rheometer from
will activate video and/or music connected to the information on Anton Paar. A cone and plate geometry (D: 50 mm, 1°) with a gap distance
the book page. The MediaBook concept is meant to be used in of 0.102 mm was used for all the measurements (environmental condition:
research on how elderly people interact with digital technology, temperature 21 ± 1 °C and RH% of ca- 45–50). The samples were pre-
sheared (1 s-1 in 60 s) before viscosity profiles were produced.
and while that research lies outside the scope of this work, the
Printing: The sensors were printed on paper sheets from Ahlström-
reader can find more information about the planned work on the Munksjö (Spantex primer foil, 120 g m−2, and SULPACK NL 41G) in a
referenced webpage.[46] Figure 5g,h shows the MediaBook being DEK Horizon 03iX flatbed screen printer and were cured in a Natgraph
used to control photograph slideshow on a computer by wireless Air Force UV Combination Dryer. The screen mesh was typically 120–34

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threads cm−1 . Carbon inks used were 7102 from DuPont, CI-2051 from Acknowledgements
EMS/Marabu and the in-house developed C:CNF ink described previously;
all inks were cured at 130 C for 90 s. in a belt oven. Dielectric patterning was The authors would like to acknowledge funding from Vinnova through the
made with UV-curable ink UVSW 170 (Marabu). The final nitrocellulose Digital Cellulose Competence Center (DCC), Diary number 2016–05193,
coating was applied by screen printing the developed nitrocellulose ink. the Swedish Foundation for Strategic Research (Smart Intra-body network;
The ink was thermally cured (120 C, 90 s) in the belt over. The nitrocellulose grant RIT15-0119), and the Norrköping municipality fund for research and
ink was applied onto the carbon in either 1, 2, 3, 4, or 5 layers. development (Accessibility and remembering – storytelling and innovative
Resistance Measurements: Sheet resistance measurements were per- media use in elderly care homes, 2020. Grant: KS 2020/0345). The work
formed on an Ossila four-point probe. The resistance limit of the measure- was also supported by Treesearch.se. The authors thank Patrik Isacsson
ment equipment was 10 MΩ sq−1 . When this sheet resistance is shown in and co-workers at Ahlstrom Munksjö for providing the paper substrates
the figures it indicates that the measured resistance was above this limit. and for valuable know-how as part of the collaboration within DCC, as well
Resistance during bending was measured using a Hewlett Packard as Erik Gabrielsson, Daniel Simon, Elisabet Cedersund, and Lars Herlogs-
32201A multimeter in a two-probe configuration. The three longest con- son for their involvement in the work on the original Mediabook platform.
ductor lines (sensors 11–13 in Figure 1) were cut out and used for the
bending tests. Bending tests were performed using a cylindric bending
tester using cylinders of different radii (between 2 and 8 mm). The effect
of the bending was evaluated by measuring the resistance of the traces Conflict of Interest
before and after each bend (starting with the largest radius). The authors declare no conflict of interest.
Triboelectric Measurements: Triboelectric characterization, that is, volt-
age response upon mechanical impact, was performed using an in-house
build setup (see Figure S4, Supporting Information). The setup consisted
of two parts, 1) A backplane mounted over a stationary base with a mi- Author Contributions
crometer screw to adjust lateral distance 2) a linearly oscillating arm. The
plate had an adhesive pad where the sensors were attached, while the mov- J.E. conceived the main idea, developed the NC-ink, assisted in the printing
able arm had a piece of leather attached to the contacting surface to simu- process, and performed the triboelectric measurements. U.L. performed
late human skin. Behind the sticky pad, a piezoelectric sensor was placed the printing fabrication and the SEM measurements. Y.M. built the tri-
to measure the impact of the arm on the sample. The triboelectric sensors boelectric measurement setup and assisted in measurements. R.B. per-
and the piezoelectric impact sensor were connected to two channels of a formed the printing fabrication and NC-ink characterization. S.P. worked
digital oscilloscope (Keysight InfiniiVision DSOX2004A) to measure the on the electronics card of the Mediabook. J.S. performed the bending tests.
generated voltage. The triboelectric sensors were also connected in par- A.F. formulated the CNF-based carbon ink. K.E., V.B., and A.A. supervised
allel to a resistor decade box to measure the generated voltage with dif- the project. All authors contributed to the writing of the manuscript.
ferent load resistance. 10 MΩ resistance was used for the measurements
unless otherwise stated. The linear actuator was connected to the function
generator of the oscilloscope allowing control of the oscillatory frequency
and waveform. 7 Hz frequency and a sinusoidal waveform were used for
Data Availability Statement
all measurements unless otherwise stated. See Figure S8 (Supporting In- The data that support the findings of this study are available from the cor-
formation) and the associated discussion in Supporting Information for responding author upon reasonable request.
more details on the choice of frequency.
Scanning Electron Microscopy: SEM was carried out with a Zeiss
Sigma 500 Gemini. The printed structures on paper were each mounted
on a carousel sample holder and grounded using copper tape. For the Keywords
carbon surfaces in Figure 4a–c, 3 eV and SE2 detector was used. For
the carbon surfaces in Figure 4d–f, 4 eV and InLens detector were used, cellulose, green electronics, printed electronics, sensors, triboelectric
except for the CNF carbon ink image that used 3 eV. For imaging of nanogenerators
the nitrocellulose coating imaging in Figure 4g–j, 1 eV and an InLens
detector were used. The SE2 detector utilized secondary electrons to Received: August 16, 2022
mainly provide information about surface topology. The InLens detector Revised: October 25, 2022
instead used backscattered electrons that gave information based on Published online: November 25, 2022
atomic weight and conductivity. In the samples here, carbon was the
main constituent in both the conducting and insulating layers. However,
insulating materials will appear dark or smooth, as seen with multiple
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