Chemical Engineering Journal 480 (2024) 147995

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Chemical Engineering Journal

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

Eco-designed recycled newspaper for energy harvesting and pressure

sensor applications
Guilherme Ferreira a, Shubham Das b, Alberto Rego a, Rafael R.A. Silva a, c, Diana Gaspar b,
Sumita Goswami b, Rui N. Pereira d, Elvira Fortunato a, Luís Pereira a, b, Rodrigo Martins a, b,
Suman Nandy a, *
a
CENIMAT/i3N, Department of Materials Science, NOVA School of Science and Technology, NOVA University Lisbon (FCT-NOVA) and CEMOP/UNINOVA, Campus
de Caparica, 2829-516 Caparica, Portugal
b
AlmaScience Colab, Madan Parque, 2829-516 Caparica, Portugal
c
Department of Materials Science and Engineering, Federal University of São Carlos, São Carlos, SP 13565-905, Brazil
d
Department of Physics and i3N - Institute for Nanostructures, Nanomodelling and Nanofabrication, University of Aveiro, Campus Universitário de Santiago, 3810-193
Aveiro, Portugal

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

Keywords: This study focuses on developing multifunctional electronic paper (e-paper) using a low-cost recycling method to
Eco-design minimize the usage of critical raw materials. The e-paper is designed for various smart applications, such as
Cellulose mechano-responsive energy harvesters and pressure sensors. The emphasis is on adopting an eco-friendly
Polyaniline
approach by utilizing cellulose extracted from used newspapers, which would otherwise have been discarded.
Energy Harvester
The formulated e-paper contains 100 % recycled cellulose fibers, unlike the more commonly used recycled paper,
Sensor
which contains around 70 % of recycled cellulose and 30 % of new pulp. The recycled paper (RP) was func­
tionalized using polyaniline (PANi), resulting in a conductive e-paper, capable of generating electric current
through a charge transfer mechanism at the PANi-Cellulose/electrode interface layer. The resulting devices
demonstrate satisfactory energy production, with output voltage ranging from 16.8 to 20.25 V, output current
ranging from 0.9 µA to 1.75 µA, and power density ranging from 0.18 to 0.35 Wm− 2. The mechanical impulses
generated by the device can successfully light up several LEDs in series. Additionally, the e-paper was investi­
gated as a flexible, paper-based pressure sensor. The fabricated device exhibited excellent sensitivity, fast
response time, and a wide detection range from 25 Pa to 12.25 kPa. The sensitivity of the pressure sensors
achieved 4.21 kPa− 1 within a low range of 0–1 kPa and approximately 0.008 kPa-1for a broader pressure range (2
– 12.25 kPa). Additionally, the durability of the pressure sensing devices has undergone rigorous testing, sur­
passing 2000 cyclic tests.

1. Introduction global environment. With the escalating consumption of electronic de­

The rapid proliferation of consumer electronics has significantly
contributed to improving living conditions for millions of individuals, as
it has effectively addressed challenges in areas such as education,
medicine, climate change, and communication technology. In fact, the
ongoing digitalization process holds paramount importance in pursuing
the Sustainable Development Goals outlined by the United Nations [1].
However, it is crucial to acknowledge the escalating impact of electronic
waste, commonly known as e-waste, on our planet. This escalating issue
demands ecological measures to prevent further deterioration of the
vices over the century, the volume of e-waste is rapidly increasing,
particularly in highly developed nations. According to the Global
Transboundary e-waste Flows Monitor 2022 published by the United
Nations, approximately 53.6 million metric tons of e-waste were
generated worldwide in 2019, with only 17 % of this quantity estimated
to have been adequately recycled in an environmentally responsible
manner. Projections indicate that this volume of electronic waste is
expected to rise by 39.4 % by 2030 and 105 % by 2050 [2]. Therefore, it
is necessary to locate sustainable material platforms to reduce the
excessive use of critical raw materials in electronic devices. Cellulose

* Corresponding author.
E-mail addresses: rfpm@fct.unl.pt (R. Martins), s.nandy@fct.unl.pt (S. Nandy).

https://doi.org/10.1016/j.cej.2023.147995
Received 22 September 2023; Received in revised form 3 December 2023; Accepted 8 December 2023
Available online 9 December 2023
1385-8947/© 2023 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC license (http://creativecommons.org/licenses/by-
nc/4.0/).
G. Ferreira et al.
substrates have demonstrated themselves to be a promising ecological
material for electronic applications such as: batteries [3,4], pressure
sensors [5,6], solar cells [7,8], and supercapacitors [9,10], amongst
others. It is well known that paper can be submitted to recycling pro­
cesses several times due to its mechanical properties. Therefore, it is
viable to implement paper in electronics as a sustainable alternative to
the materials more commonly used nowadays.
However most electronic applications comprising cellulose are
mostly focused on using cellulose derivatives or polymorphs like cellu­
lose nanocrystals (CNCs) and nano- and micro-fibrillated cellulose
(NFCs and MFCs). These require a high level of processing and the use of
raw materials. There is still little focus on the use of recycled paper for
electronic applications. Table S2 in Supporting Information presents
some recent works based on recycling of wastepaper for different elec­
tronic applications. Recycling strategies for recovering or re-
implementing paper-based materials into new devices require careful
consideration, as recycling can be energy-intensive depending on
product complexity. Reusing materials, on the other hand, is environ­
mentally preferable, involving no additional treatment. Recycling
newspaper or used paper for smart applications poses challenges related
to cost-effective functionalization, device stability, and efficiency. In
this respect this reported works have made valuable contributions, the
current study seeks to distinguish itself by employing a low-cost recy­
cling method to develop multifunctional electronic paper (e-paper) with
a focus on minimizing the use of critical raw materials. The novelty of
such an approach lies in adopting an eco-friendly strategy by utilizing
100 % recycled cellulose fibers extracted from used newspapers. This
stands in contrast to conventional recycled paper, which often comprises
a lower percentage of recycled cellulose (less than 70 %).
Herein, we have developed recycled newspaper cellulose substrates
with an environmentally friendly eco-design for energy harvesting and
pressure sensor applications with good mechanical stability. Adopting
this ecological approach to energy science requires substituting con­
ventional materials with new functional “green” materials that offer
superior mechanical, electronic and socio-economic advantages. Addi­
tionally, the recyclability of used newspaper presents a promising op­
portunity to replace the excessive and costly use of new raw materials in
previous investigations on pressure sensors [11–16]. While these studies
have reported impressive sensing performance, the limitation lies in
their ability to be fabricated on a large scale due to the use of non-
renewable materials. Consequently, the production of cellulose-based
sensors is gaining momentum, primarily because of their abundance
and conductivity performance. Additionally, our investigation extends
to the application of the developed e-paper as a flexible, paper-based
pressure sensor, demonstrating excellent sensitivity and response char­
acteristics within a wide working range.
During this work, we investigated the functionalization of recycled
cellulose paper substrate with polyaniline (PANi), through an in-situ
polymerization technique, for electronic applications. PANi falls into
the category of conjugated polymers. These are organic macromolecules
with de-localized π-electrons arising from overlapping of p-orbitals,
which have been shown to have numerous smart electronic applications
namely: mechanical energy harvesting [17,18], batteries [19,20],
supercapacitors [21,22], transistors [23,24], etc. PANi has a wide-range
of applications in organic electronics due to its ability to control its
electronic and chemical properties by recurring to doping-dedoping
strategies to tune its electronic properties, introducing ionic com­
pounds in its nanostructure. The eco-design strategy for energy har­
vesting and pressure sensor devices will involve functionalizing the
recycled newspaper cellulose fibers with PANi and coupling with a
paper-based electrode. Charge transmutation will occur from the poly­
meric layer (charge transfer layer, i.e., CTL) to the metallic one (charge
collector layer i.e., CCL). When a pressure is applied onto the surface of
the device, there will be an increase of localized charge density due to
the nanoscale bending of the PANi polymeric chains, causing a Fermi-
level pinning and a consequent transfer of charges to a more stable
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Chemical Engineering Journal 480 (2024) 147995
energy state in the metallic layer. When stress is released, the polymeric
chains will regain their original structure and create a region with
shortage of charge-carriers, which will be balanced with charges from
the nearby networks, enabling a new pressure-release cycle [25,26].
2. Materials and methods
To produce the cellulose samples three main reagents were consid­
ered that were used differently depending on the sample: sodium chlo­
ride (NaCl; ≥99.0 %, ACS reagent, Sigma-Aldrich), citric acid (CA; 99.5
%, Sigma-Aldrich), and sodium dodecyl sulfate (SDS; ≥99.0 %, ACS
reagent; Sigma-Aldrich).
Meanwhile, for the synthesis of PANi, to functionalize the samples,
the following reagents were used: aniline (AN; 99.5 %), ammonium
persulfate (APS; 98.0 %), camphor-10-sulfonic acid (CSA; 98 %, Sigma-
Aldrich) and hydrochloric acid (HCl; ≥37 %, Sigma-Aldrich).
All the recycling and functionalization methods were carried out in a
low-cost technique. Furthermore, for smart device applications, screen
printed silver layer has been used as an electrode layer.
2.1. Recycling of the newspaper
Used newspapers were recycled as the main substrate through a se­
ries of simple procedures. Initially, the newspapers were cut into small
pieces and soaked in deionized water (DI water) to facilitate the sepa­
ration of fibers. The resulting paper pulp was obtained by pouring the
mixture and excess water was removed using an 800 μm drainer to
prevent pulp loss. The pulp was further processed by forming small
pieces, which were then squeezed, cut, and dried in an oven at 60 ◦ C for
24 h. After drying, the pulps were blended again to obtain small flakes,
referred to as recycled cellulose fibers, which were subsequently used in
the samples. To disperse the cellulose fibers in 160 ml of DI water, a
blender was utilized, and ultrasonic liquid disperser (Sonics VCX 750,
13 mm) was employed to ensure efficient fiber separation. During this
process, the solution was continuously stirred at 500 rpm and main­
tained at room temperature. After filtration, the cellulose fibers were
transferred to polystyrene Petri dishes with an approximate volume of
43 cm3, which were reused for this purpose. Subsequently, the samples
were dried in a laboratory oven at 60 ◦ C for 24 h. Once the paper was
completely dried, all samples were removed from the Petri dishes and
subjected to further characterization.
2.2. Functionalization of recycled paper
For the synthesis of PANi, the reagents that have been used are
mentioned in the main body of the text. The synthesis of the Emeraldine
state of PANi, requires two solutions (oxidizing solution: solution A and
monomer solution: solution B). The oxidizing solution was prepared
with 0.928 g of APS dissolved in 10 ml of DI water and the monomer
solution, with 0.4646 g of CSA dissolved in 20 ml of DI water. After 10
min of steering agitation (450 rpm) of both the solutions, 100 μl of HCl
and 365 μl of Aniline were added to solutions A and B, respectively. The
solution was then mixed agitated again for 10 min to homogenize the
chemicals before the functionalization of RP. The oxidizing and mono­
mer solution were added together for the polymerization from aniline to
polyaniline. After mixing both samples, it took around 5 min for them to
change into the desired color (dark greenish blue indicating the poly­
aniline phase). All the RP samples were immersed into that solution for
2 min to functionalize the sample. The functionalized RP (RFP) was then
dried at room temperature and prepared for chemical analysis and de­
vice fabrication.
2.3. Fabrication of electrodes
The flexible electrodes layers for the smart device’s fabrication were
produced by screen-printing, using silver ink (CRSN2442 AG INK,
G. Ferreira et al.
Coated Screen Inks). The ink was printed on Whatman paper (What­
manTM, Chromatography Paper, Grade: 1CHR) for fabricating several
electrodes, and dried on a hot plate at 100 ◦ C for about 30 min. These
electrodes were integrated into the cellulose-PANi based device as a
charge collector layer.
2.4. Fabrication of the devices: Energy harvester and pressure sensors
The paper-based devices were designed with the RFP as active layer
(AL) and screen-printed Ag electrode as charge collector layer (CCL).
The AL was connected directly to the CCL on both surfaces; also, two
copper tapes were connected on each side as extended electrodes to
prevent damaging of the CCL during handling or measurements. All the
layers are fixed with commercial tape, to provide the necessary stabili­
zation to the device. All the devices were of the same size and shape,
with a 4 cm2 AL.
2.5. Characterization Techniques: Morphological, compositional and
electrical characterization
Several characterization and analytical tools were used to determine
the samples’ morphological, chemical, and compositional properties
before and after functionalization. The morphological analyses of the
cellulose fibers were made by a field emission scanning electron mi­
croscope (FESEM, Hitachi TM3030 Plus) while the elemental
Fig. 1. (a) Schematic of the process for obtaining the recycled cellulose fibers from the newspaper; (b) Schematic of the process used to transform the recycled
cellulose fibers into recycled paper substrate. (c) Schematic of the functionalization process of RP with PANi; (d) Surface resistance observed for e-paper, showing an
increase in conductivity from the unfunctionalized RP samples.
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Chemical Engineering Journal 480 (2024) 147995
composition of the samples was analyzed via energy dispersed X-ray
spectroscopy (EDX, Oxford INCA Energy 350).
Fourier-transform infrared spectroscopy (FTIR, Thermo Nicolet 6700
Spectrometer) was used for chemical analyses of the samples, before and
after polymerization. Attenuated total reflectance (ATR) was applied in
a spectral range (wavenumber) between 500 and 4500 cm− 1. The
electrical characterization of the polymerized samples was conducted
using a Hall effect system to measure the functionalized samples’ sheet
resistance and hall mobility. Meanwhile, the mechano-electrical char­
acterization of the energy devices was done by measuring the mechan­
ical impulses generated on the device with the assist of a standard
oscilloscope (Tektronix TBS 2022). The voltage values obtained from the
mechanical pulses were later transformed into current and power den­
sity values. The analytical data from the resistive pressure sensors were
recorded through Arduino-customized electrical measurement setup
system.
3. Results and discussion
3.1. Fabrication of the recycled paper (RP) samples and recycled
functionalized paper samples (RFP)
This study aims to develop a cost-effective method for recycling
newspaper into recycled cellulose paper pulp. The focus is on creating a
new paper substrate exclusively from 100 % recycled cellulose material
G. Ferreira et al.
without incorporating any binder elements. The aim is to provide a
sustainable and eco-friendly paper substrate for electronic applications,
promoting circular economy principles and reducing environmental
impact. In this study, old newspapers were subjected to a series of
chemical processes to produce recycled paper substrates (RPs), followed
by polymeric functionalization. The schematic illustration of the recy­
cled cellulose fiber-making process from used newspaper is depicted in
Fig. 1(a). The recycled paper substrates were prepared into profuse
layers structure using sodium dodecyl sulfate (SDS). The usage of SDS
targeted improving the porosity of cellulose matrices by forming the
foam during the chemical process [27]. Citric acid (CA) was used during
the paper fabrication method to increase the stability and strength of
cellulose materials by increasing the cross-linking between the cellulose
fibers networks and strengthening them [28,29]. Moreover, sodium
chloride (NaCl) was also used to act as a bonding agent between the
cellulose fibers and the reactants [30,31].
Fig. 1(b) shows the schematic preparation flowchart of the RP
fabrication method, as well as a snapshot of the fabricated RP. The
standard paper recycling protocol was adapted using 3 w/w% of recy­
cled cellulose to optimize the paper-making process [32]. Nevertheless,
while using this percentage it was verified that the pH level (pH = 6.5)
was not decreasing as expected with the addition of CA. This is probably
due to a low chemical bonding since the cellulose samples had a high
concentration of lignin and fillers. By reducing the quantity of cellulose
to 1 w/w%, the pH had decreased to 3.5, but the fabricated RPs were still
rigid and easily breakable. With further decrease of cellulose fibers
concentration to 0.5 w/w% and 0.2 w/w%, it was verified that the first
one presented exceptional flexibility, adequate sponginess, and a
smooth surface, while the 0.2 w/w% one was too fragile and therefore
discarded. After the chemical optimization process, three different types
of recycled paper substrates were analyzed.
PANi was chosen as the conjugated polymer to enhance the func­
tionality of the recycled paper (RP) samples. This selection was based on
several factors, including the ease of synthesis, widespread availability,
and the ability to finely tune its properties through ionic doping and de-
doping strategies. The decision to utilize PANi in the functionalization
process aims to capitalize on its advantageous characteristics, facili­
tating the development of tailored properties and improved perfor­
mance in the RP samples for desired electronic applications [33]. The
synthesis of PANi involves the preparation of two precursor solutions: an
oxidant solution and a monomer solution. The oxidant solution
comprised hydrochloric acid (HCl) and ammonium persulfate (APS)
dispersed in deionized water. The monomer solution consisted of a
mixture of camphor-10-sulfonic acid (CSA) and aniline monomer (AN).
The AN monomer is a neutral entity, that in the presence of APS, which
acts as a redox initiator, will form benzenoid rings linked together with
amine groups (–NH–) and quinoid rings bonded together with imine
moieties (–N = ), due to the delocalization of two electrons [34,35]. The
quantity of APS added to the mixture will influence the phase of PANi
obtained in the functionalization. There are three different phases of
PANi: leucoemeraldine, (the fully reduced polyaniline state), which is
non-conductive and colorless; pernigraniline (the fully oxidized poly­
aniline state), which is a dark blue/violet insulating polymer, and
emeraldine, which has equal quantity of reduced and oxidized monomer
[36–38]. It is important to synthesize emeraldine due to its semi-
conducting properties [39]. Additionally, the conducting properties of
the emeraldine state of PANi are increased with the protonation of the
entity with aqueous HCl [40]. The amine groups present in the network
of PANi will interact with HCl, by dropping one of the electrons from the
nitrogen lone pair and consequently forming a polaron conduction band
[41]. The CSA was added to act as a co-doping agent increasing the
conductivity while providing a hydrophobic component. The hydro­
phobic component comes from the micelle structure of the CSA and will
prevent moisture from influencing the deprotonation of the polymeric
chain. Fig. 1 (c) presents a schematic of the fabrication of RFP samples.
Firstly, both solutions are prepared and kept under an ice bath for 30
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Chemical Engineering Journal 480 (2024) 147995
min, to bring their temperature down. The two solutions are then mixed
together, with mechanical agitation until the proper homogeneity of the
new solution is assured.
The new polymeric solution must be placed rapidly in an ice-bath to
slow down the polymerization reaction, which will ensure the formation
of longer and more stable polymeric chains, resulting in higher con­
ductivity and less chaotic agglomeration of microstructures. The solu­
tion is left in the ice-bath for the next 30 min and a new dark greenish
blue colour, which indicates the presence of emeraldine phase of PANi,
starts to show. The RP samples are then immersed into said solution for
2 min for functionalization and then left to dry at room temperature for
24 h. The conductivity of the samples increased as a result of the poly­
meric functionalization. Recycled functionalized paper (RFP) samples
had a surface resistance in the 1–4 kΩ range, as shown in Fig. 1 (d) for e-
paper (PANi functionalized paper).
Fig. 2 presents the morphological cross-sectional (Fig. 2 (a-c)) and
top view (Fig. 2 (d-f)) images of all prepared RP samples with a snapshot
of each paper sample. RP1 and RP2 have more gaps between the fiber
walls as well as more dispersion and lost fibers. In RP1, that could be
explained by the absence of any other chemicals, especially CA, which
strengthens the cellulose networking; whereas in RP2 it could be
explained by the absence of NaCl, which allows for a better bonding of
the SDS (Sodium dodecyl sulfate, foaming agent) with the cellulose fi­
bers. Table 1 briefly describes the chemical reagents used for each
sample RP1, RP2 and RP3, as well as their thickness, density, and
porosity.
Similar morphological analysis was also done in the RFP samples as
shown in Fig. 2 (g-i). Based on the photographic images, a clear and
uniform dark green color observed throughout the sample indicating
that RFP3 achieved superior superficial and internal functionalization
compared to other samples. SEM images revealed a granular structure
consistent with PANi, which is a common configuration observed in
cellulose fibers microstructures [42–44]. These observations suggest
that the functionalization process using PANi was successful, leading to
enhanced properties and a more uniform distribution of PANi within the
recycled paper material. The reaction parameters are the main players in
shaping the microstructures. Most notably, the presence of CSA gives the
molecules its amphiphilic configuration.
ATR-FTIR spectra of the corresponding samples are shown in (Fig. 2
(j-l)), where different peaks can be retracted and analyzed. To observe
the changes in specific patterns of the chemical composition of the
samples, before and after functionalization, all of them were analyzed on
ATR-FTR. Two bands that confirm the presence of cellulose, which can
be observed on both spectra of the recycled wastepaper: The peak of the
C–H stretching vibrations (~2900–2905 cm− 1) due to the general
organic content present on the samples, and the peak of the C–O–C band
and C–C ring breathing (~1145–1152 cm− 1) authenticate the presence
of cellulose fibers on the recycled paper on both phases [45]. Although
these peaks are observed on both phases, the peaks intensity after
polymerization decreases since most of the cellulose fibers are covered
with polyaniline, lowering the values of cellulose detected from the
reflected IR spectra. When analyzing the spectra generated by PANi
(Fig. S2(b) in Supporting Information), typically five peaks stand out
compared to the pre-functionalized paper. The peak at ~ 800–807 cm− 1,
C–H bond, manifests the benzene circle of PANi stretching vibrations
and the peak of ~ 1100–1124 cm− 1 represents the quinoid band, –N = Q
= N–, stretch vibration. The C–N bonds with peak at ~ 1304–1307 cm− 1
corroborate the stretching of the benzenoid rings of PANi [46]. At last, C
= C bands are spotted on both curves with two peaks between ~
1480–1488 and ~ 1565–1580 cm− 1, which indicates the presence of
lignin on the fibers of the wastepaper and the stretching of the quinoid
and benzenoid rings in the doping of the conjugated polymer [47].
Additionally chemical and morphological analysis of pristine PANi
nanostructures by FESEM, FTIR and TEM with EDS mapping has been
shown in Figs. S2 and Figs. S3 in Supporting Information.
G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

Fig. 2. Morphological images of three types of recycled paper samples. The cross-sectional SEM images have been shown for sample (a) RP1, (b) RP2, and (c) RP3,
respectively; The top view surface morphological images of corresponding samples shown in (d) RP1, (e) RP2 and (f) RP3, respectively. FESEM surface morphology
analysis of RFP samples (g) RFP1, (h) RFP2 and (i) RFP3 respectively with a snapshot image of the correspondent sample (inset); Comparison of ATR-FTIR spectra
curves before and after functionalization of each sample; Spectra of pristine and PANi functionalized samples: (j) RP1 and RFP1 spectra with the PANi bands and
correspondent designation (same on the other graphs); (k) RP2 and RFP2; (l) RP3 and RFP3; The dashed lines are indicating the position of the characteristic PANi
absorption bands present for every RFP sample spectrum.

3.2. Cyclic compression test
Cyclic compression tests (SHIMADZU, EZ Test, Table-Top Tensile
Tester), spanning 100 cycles, were conducted on both PANi-
functionalized paper i.e., e-Paper and the pristine recycled paper to
examine their mechanical performance and stability (Fig. 3). The cyclic
compression test, extending up to 80 % strain, validated the enhanced
mechanical resilience of e-Paper (sample code: RFP3) compared to
recycled paper (sample code: RP3). This was evident because RP3 did
not withstand 80 % compression, hindering data collection, while the e-

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G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

Table 1
Brief description of chemical reagents with the physical properties of as-fabricated three different types of RP samples.
Sample Cellulose (g) Citric Acid (g) SDS (g) Sodium Chloride (g) Thickness (µm) Density (g/cm3) Porosity (%)

RP1 0.83 – – – 722 0.27 83.1

RP2 0.83 0.25 0.015 – 871 0.22 86.3
RP3 0.83 0.25 0.015 2.922 g (5 ml of DI water) 1261 0.31 84.5

Fig. 3. Cyclic compression test of 100 cycles at 20% strain for recycled paper (RP3) (a), e-Paper (RFP3) (b), and at 60% strain for sample recycled paper (RP3) (c), e-
Paper (RFP3) (d), respectively. Maximum stress (e), and Young’s modulus (f) obtained at different strains for recycled paper (RP3) and e-Paper (RFP3). The shaded
portion indicates that the Young’s modulus stable after 20 cycles.

Paper could bear at least 100 cycles of mechanical compression.
In the initial compression, both materials exhibited linear elastic
responses at low strains, i.e., 20 % of strain (Fig. 3 (a,b)). The elastic
behavior ceased around 1.06 and 0.12 kPa for RP3 and RFP3, respec­
tively. The transition from elastic to plastic behavior was less apparent
at lower strains (20 % and 40 %), becoming more pronounced at 60 %
and 80 % strains, indicating non-linear behavior and the initiation of
plastic deformation. Cyclic compression at 60 % strain led to the rupture
of chemical bonds, resulting in material degradation and reduced energy
absorption (Fig. 3 (c,d)). Even after 20 cycles at 60 % strain, the loading
and unloading curve failed to align with the initial curve, signifying
material degradation (Fig. 3 (c,d)). At 20 % strain, the cyclic compres­
sion curves retained better overlap over in the initial 20 cycles, con­
firming the material’s elastic limit at around 20 %. Additionally,
comparison of the recycled paper and e-Paper under different strains
during the compression test has been shown in Fig. S5 (Supporting
Information).
PANi functionalization resulted in reduction of the maximum
compressive strength from 45.5 to 22.9 kPa after 60 % strain, consid­
ering the first cycle of compression (Fig. 3 (e)). Both samples experi­
enced a reduction in maximum compressive strength (approximately
43.5 and 10.6 % for e-paper and paper, respectively) after 100 cycles,
attributed to mechanical fatigue. Similarly, the stiffness (Young’s
Modulus) of e-paper decreased by up to 66.5 % after PANi functionali­
zation, from 0.15 to 0.05 kPa (Fig. 3 (f)), behavior also observed by
Rizvi, et al. [48]. This decline in mechanical performance is explained
by the reduction of hydrogen bond formation between cellulose
microfibrils due to modification by PANi [49,50].
Through a correlation analysis between the maximum compression
resistance exhibited by the RFP3 paper (Fig. 3 (e)) and the sensitivity of
the pressure sensor (Fig. 6 (b)), it is expected that the sensor manifests
prolonged durability when employed for monitoring at low pressures
(<0.71 kPa). This extended service life is attributed to the RFP3 paper at
pressures within the elastic deformation range of e-paper, resulting in
reduced degradation over time. Additionally, heightened applied pres­
sures correspond to increased compressive strength in the material,
indicating polymer densification. In essence, compressing the material
from 60 to 80 % necessitates 40 % more force compared to the force
required for compression from 40 to 60 %, revealing that the fibers are
really very compacted, leaving very minimal void spaces within the
RFP3 paper. Furthermore, the material stiffness significantly decreased
in the initial cycles, indicating rupture of polymer bonds, stabilizing
after the 20th cycle.
3.3. Recycled paper for energy harvesting application
The prototype energy harvester devices were fabricated using the
RFP samples as the active layer (AL), clipped with two electrode layers,
which act as a CCL as shown in Fig. 4 (a). Silver (Ag) screen printed
paper (commercial Whatman paper grade 1) was used as CCL. All the
energy harvesting devices were built using this configuration, with 4
cm2 of area and Ag electrode as CCL material. Screen-printed Ag was
chosen because the difference between the work function of PANi and
Ag is the lowest compared with other available electrode materials such

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G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

Fig. 4. (a) Schematic of the energy harvesting building block architecture, comprising an active layer and two silver paper-electrode layers; (b) Schematic of the
charge transfer mechanism responsible for the generation of an output voltage; when pressure is exerted, localized charge density is increased due to mechanical
impulse which initiates charge translocation between polymer/electrode interfaces and initiate current flow. When pressure is released, charge scarcity appears into
the deformed polymeric network that are reinstated by neighboring free charge carriers in the polymeric network allowing the next pressure cycle. Open circuit
output voltage (Voc) is shown for each three types of device (c) RFP1 (d) RFP2 and (e) RFP3. The corresponding short circuit output current (ISC) is shown in (f)-(h),
respectively. All the output performances were obtained using the same force and frequency (12 N, 5 Hz).

as carbon, copper (Cu) or aluminum (Al) [18].
The energy harvesting mechanism employed in this study is based on
applying a mechanical stimulus to the device’s surface, resulting in a
physical deformation of the polymeric network. This deformation causes
the polymeric chains to become more compacted, increasing local
charge density concentration. As a consequence, a Femi level pinning
occurs, initiating a charge transfer mechanism. During the charge
transfer process, charges are transmuted from the localized pressured
area of the AL to the more stable energy levels of the CCL. Upon
releasing the pressure, the elastic behavior of the polymeric chains
causes the polymeric structure to revert to its original configuration.
This re-expansion of the polymeric chains leads to a scarcity of charge
density in the previously pressurized region. To compensate for this,
charges from neighboring regions with higher carrier density trans­
locate, neutralizing the entire polymeric structure. This dynamic process
enables a continuous and cyclical pressure-release cycle, facilitating
repeated energy harvesting from mechanical stimuli. The demonstrated
charge transmutation and redistribution within the polymeric network
underline the feasibility and efficiency of the energy harvesting
approach based on the polymeric network’s elastic behavior and charge
carrier dynamics. A schematic of the mechanism is depicted in Fig. 4 (b).
All the devices underwent a comprehensive comparative analysis based
on their open-circuit output voltage (Voc) and short-circuit output cur­
rent (Isc), as illustrated in Fig. 4 (c)-(h). To measure Voc, the device’s
output was directly connected to an oscilloscope. For Isc measurement, a
customized short circuit setup comprising a bridge rectifier and a load
resistance was employed to facilitate accurate current calculation before
connecting to the oscilloscope. The obtained Voc values for all devices
showed no significant variation, falling within the range of 16.8–20.25
V. Notably, the output current exhibited considerable variation among
the energy devices, ranging from 0.9 µA to 1.75 µA, depending on the
specific type of recycled paper substrate utilized. The energy device
made from RFP1 sample shows the lowest Voc and Isc of 16.8 V and 0.89
µA respectively, whereas the energy device from sample RFP2 shows an
increment of Voc and Isc, having values of 17.5 V and 1.16 µA respec­
tively. The energy devices made from RFP3 samples show the highest
output voltage and current, averaging 20.25 V and 1.75 µA, respectively.
The different electrical output is due to the recycling process of the
paper substrate. On the other hand, interestingly, it can be noticed that
the increment of the output current is much higher than the increment of
the voltage. For example, from sample RFP1 to RFP2, the Voc increased
4.2 % where the Isc increased 38 %. The trend is similar from sample
RFP2 to RFP3, where the increment of Voc and Isc are around 15 % and
40 % respectively. It is quite an interesting observation because high

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G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

impedance nanogenerator generally shows higher voltage than current cycles. Moreover, capacitor charging test was performed using different
output increments. From Table 1 it can be noticed that with different types of capacitors. Fig. 5 (f) shows the capacitor charging test from the
reagents and processes, the thickness of the recycled paper substrate most efficient energy device of RFP3. The device was able to charge
increased from RP1, to RP2 and RP3. Despite using the same amount of different commercial capacitors with the capacitance value of 0.1µF,
cellulose for all, due to the increment in thickness the porosity of the 0.22 µF, 0.47 µF and 1 µF up to 1 V in 6, 7.5, 8 and 42.5 s, respectively.
recycled paper substrate also increased, which in turn may increase the The relationship between capacitance and energy stored can be defined
loading of PANi nanostructure during functionalization causing lower through the following equation:
impedance of the AL. Moreover, the highest electrical performance of
CV 2
the RFP3 sample is anticipated because of its stable chemical cellulose E= (3)
structure, the bonding properties of the NaCl, and the presence of Cl-
2
ions in the structure. The mechano-responsive electrical outputs of the Wherefrom we can derive that the energy accumulated in a 1 µF
devices corroborate the chemical and morphological analyses of the capacitor is 50 × 10-8 J in 45 s. The energy accumulated in the other
recycled paper samples. When comparing the electrical performance of capacitors are: 5 x 10-8 J, 11 × 10-8 J and 23 × 10-8 J, for 0.1µF, 0.22 µF
the samples, the resistance and mobility mirrored the performance of the and 0.47 µF, respectively. The relationship with power can be obtained
devices in general (Table S1). The force applied during the measure­ through:
ments was taken using a commercial pressure sensor (FSR 406), whereas P = Et (4)
the frequency was analyzed with the periodicity of the voltage peaks.
Wherefrom we can get the direct instantaneous power of the sensors.
Furthermore, the power and current density of the devices were
The direct power of the sensor was calculated as an average of the power
analyzed across the different load resistances from 100kΩ to 100MΩ
obtained for all the capacitors obtained: 8 × 10-9 W, 15 × 10-9 W, 29 ×
(were added in series on a rectifier circuit), so that the performance
10-9 W, and 12 × 10-9 W for the 0.1µF, 0.22 µF, 0.47 µF and 1 µF,
concerning different loads could be evaluated. The current and power
respectively, resulting in an average power of 16 × 10-9 W.
density were evaluated for the area of the devices (4 cm2). The scattered
values presented for each resistance result from the average peak
voltage values obtained in the oscilloscope which were then converted 3.4. Recycled paper for pressure sensing and IoT application
to current density and power density.
Recently, the application of conductive paper-based materials has
V
I= (1) been quickly evolving in wearable electronics. Nonetheless, recycled
R*A
paper for electronic applications contains only 70 % recycled paper,
V2 needing 30 % of new pulp in its formation [51]. The sensing prototypes
P= (2) fabricated herein use 100 % of recycled paper in its structure. The
R*A
pressure sensing devices were designed in a sandwich structure, with
In Table 2, it is represented the typical characteristics obtained for two screen-printed silver electrodes paper substrates and in between the
each device including Voc, Isc, maximum power density (Pmax) and cur­ RFP samples, as depicted in Fig. 4 (a). Here, the sensor works on the
rent density (Imax). resistive mechanism, where the internal resistance of the devices
The power density curves follow the same pattern as the Voc and Isc changes with the pressure applied onto the surface. The pressure sensor
curves, where RFP1 presented the lowest value of Pmax (0.18 W m− 2) measurements were conducted on an Arduino platform. A voltage
and device RFP3 achieved the maximum value of 0.35 W m− 2 for Pmax. divider circuit was designed to assist in the measurement of the internal
Also, device RFP3 achieved the highest Imax value of 32.9 mA m− 2. The resistance of the pressure-sensing devices. The circuit consisted of a
results corroborate the most homogeneously functionalized material constant voltage source provided by the Arduino platform in series with
with polymer microstructures of PANi observed in SEM. The power and a bridge rectifier, a load resistor (100 kΩ) and the pressure sensor. A
current density curves are depicted in Fig. 5 (a)-(c). constant voltage source of 5 V feeds the circuit allowing current to flow
The energy harvesting devices fabricated in this study were utilized through the device. By applying pressure on top of the sensor, the
to power a series of LEDs in a specific circuit configuration, as depicted cellulose-polymeric network became condensed, decreasing sensor’s
in Fig. 5 (d). Additionally, a visual representation of the illuminated internal resistance, hence resulting in a decrease of voltage drop across
LEDs can be observed in Fig. 5 (e). The circuit configuration involved the sensor. When pressure is released, the cellulose-polymeric network
connecting the LEDs in series with a bridge rectifier, responsible for returns to its primary internal resistance (higher than the deformed
converting the negative output to a positive one and coupling them with condition), resulting in a high voltage drop across the sensor. The sensor
the energy harvesting devices. This experimental demonstration un­ detected variances of pressure between 12.25 kPa and 0.12 kPa, for
derscores the capability of the energy harvesting devices to effectively several loading cycles, as shown in Fig. 6 (a). Interestingly, the per­
power the LEDs through the cyclic application of mechanical pressure. centage of variation in voltage dropped across the sensor is dependent
The intermittent illumination of the LEDs aligns with the dynamic na­ on the applied pressure range. Hence, the sensor’s sensitivity is highly
ture of the energy harvesting mechanism, wherein mechanical stimuli dependent on the applied pressure region.
result in charge transfer and subsequent illumination, and the subse­ The performance of the sensor can be defined as the change in the
quent release allows the system to reset for further energy harvesting sensors internal resistance, observed through voltage (ΔV) as a result of
the pressure being applied (ΔP), and through the sensitivity (S) curve
which represents the slope of the sensors internal resistance with the
Table 2
applied pressure:
Electrical output performance obtained from three different energy harvesting
devices. ΔV
S=( )/ΔP (5)
Sample Sheet Open Short Max. Current Vo
ID Resistance Circuit Circuit Power Density,
(RSH) (Ω. Voltage, Current, Density, Imax (mA Fig. 6 (b) exhibits the sensitivity curve from the complete range of
cm− 2) Voc (V) Isc (µA) Pmax (W m− 2) applied pressure values from 12.25 kPa to 0.0025 kPa. Due to its
m− 2)
nonlinearity nature, the sensitivity of the devices is calculated for three
RFP1 3180 16.8 0.89 0.18 18.5 different pressure regions: Region 1 and Region 3 comprised below 0.01
RFP2 2870 17.5 1.16 0.25 25.5 kPa pressure (lower pressure region) and above 2.45 kPa pressure
RFP3 670 20.25 1.75 0.35 32.9
(higher pressure region) range, respectively. Region 2 comprised

8
G. Ferreira et al.
Fig. 5. Current and power density for different load resistances applied in series to the device. These results were achieved due to output voltage from mechano-
responsive stimulus on each RFP energy devices: (a) RFP1; (b) RFP2; (c) RFP3; (d) Schematic of the circuit used to light LEDs and snapshot of the real-life circuit and
(e) LEDs lighting up with energy provided by the eco-energy harvesting devices; (f) Direct capacitor charging performance with energy harvesting device based on
RFP3 for different capacitors.
between 2.45 and 0.01 kPa pressure (medium pressure region) range.
The calculated sensitivity was found to be, 0.008 kPa− 1 for the higher-
pressure region, 0.29 kPa− 1 for the mid-pressure region, and 4.91
kPa− 1 for the lower-pressure region with a good-of-fit measure linear
regression model (R2 > 0.99). The fitting curve is shown in the sup­
porting information. The higher sensitivity observed in the lower pres­
sure range can be attributed to the softness of the RFP sample fibers and
the air gaps inside the structure, allowing for ease of deformation in the
low-pressure region. Initially, as pressure increases, the small weights
affect the superficial air gaps, leading to the first stage of behavior
deformation. In the second stage, there is more resistance from the RFP3
fibers, and while air gaps are still present, it becomes increasingly more
difficult to deform the structure due to the fibers being more tightly
compacted. Finally, in the third stage, the porous structure of the RPF3 is
significantly compressed, with very few air gaps and very tightly com­
pacted fibers. Further structure compression requires increasingly
higher pressure to observe any output variations, representing the re­
gion with the lowest sensitivity. The response and relaxation time of the
sensor are 129 ms and 145 ms, for a pressure of 5 kPa. The sensor’s
response time and relaxation time were measured as 129 ms and 145 ms,
respectively, at a pressure of 5 kPa. The response time was shorter than
the relaxation time, which can be attributed to reconstructing the
compressed functional cellulose structures to their initial configuration.
Upon applying pressure, the functional cellulose structures undergo
compression, leading to a change in their physical properties. As pres­
sure is released, the cellulose structures gradually return to their original
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Chemical Engineering Journal 480 (2024) 147995
state. This reconstruction process involves the reorganization of mo­
lecular arrangements and the restoration of the material’s initial
morphology. The observed phenomenon, where the response time is
shorter than the relaxation time, is consistent with expectations. After
the pressure is released, the reconstruction process requires slightly
more time to complete, resulting in a longer relaxation time than the
time taken for the material to respond to the applied pressure. These
findings highlight the dynamic behavior of the functional cellulose-
based sensor, indicating its ability to detect changes efficiently and
promptly.
In this study, we present the performance of a pressure sensor made
from recycled cellulose and PANi as the sensing material. The senor’s
sensitivity was found to be in the range of (0.008 – 4.91) kPa− 1. The
sensor could detect pressures in the range of 0–12.5 kPa. Besides, this
work investigates a new sensor design made with 100 % recycled
newspaper. While comparing its performance with previously published
works, our results show higher sensitivity, detection range, and response
time compared to Zheng et al., [52] reporting on PANi/PDMS compos­
ites and Arias-Ferreiro et al. [53] who reported on a PANI-Lignin filler
for acrylic composites. Similarly, the sensitivity and detection range of
our sensor were found to be lower than those reported in Zheng et al.
[54], on a 3D cracked PANi/PDMS foam with sensitivity of
(0.0027–0.055) kPa− 1, and detection range of (0–5) kPa. The higher
sensitivity can be attributed to a higher softness and porosity of the RP
samples. The air gaps allow for easy variation of the foamy structure
with small pressures. In contrast the detection range can be attributed to
G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

Fig. 6. (a) Response of the pressure sensing device with RFP3 paper under different pressure variations, ranging from 0.12 kPa to 12.25 kPa; (b) Sensitivity and ΔV/
V0 verified for RFP3 pressure sensor device under several loads; (c) Response and recovery time of pressure sensor with RFP3 at 5 kPa.

a smaller thickness of the sample reported (200–300) µm, allowing for
fewer fiber compression and voltage variation. The smaller response and
recovery time is due to a smaller air gap in the structure, resulting in
faster fiber compression. In contrast, the sensor reported by Chen et al.
[55], which utilized PANi functionalized cotton fibers with Ni and Cu
films, showed higher detection range, yet lower sensitivity
(0.0053–0.11) kPa− 1. The lower response time and recovery in our
sensor is likely due to our RFP samples’ foamy structure when compared
to cotton fibers. The RFP sample has air gaps making deformation
longer, which justifies the higher sensitivity in the low-pressure range,
being more prone to small pressure changes. Kannichankandy et al. [56]
reported on a pressure sensor based on a PANi functionalized commer­
cial cellulose, which reported higher sensitivity but lower detection
range in the lower regions. The commercial cellulose is less foamy than
the RFP samples, which do not allow for precise detection of pressures in
the lower regions. Nevertheless, our study shows more promising results
using 100 % recycled newspaper as a sustainable and cost-effective
material for sensor design in smart packaging applications, while
further optimization of the thickness and structure may improve the
sensitivity and detection range of the sensor. Response time is likely to
be improved as well with the detection range. Table 3 compares the
recently reported PANi based pressure sensor with our work.
To further infer the stability of the device, we have performed cyclic
compression tests on the sample RFP3 for 2 different pressures (1.23 and
5 kPa), where the pressure was applied periodically on the sensor for
1000 cycles for each case (as shown in Fig. 7). Fig. 7 (a) represents the
data taken for 1.23 kPa pressure (Blue curves) and Fig. 7 (b) for 5 kPa
(Red curves). Two different magnified ranges (one close to 100 cycles

Table 3
Comparison of the performance of the recently reported polyaniline-based pressure sensor with RFP3 pressure sensor.
Materials/Device Structure Sensitivity (kPa¡1) Response Time (ms) Recovery Time (ms) Detection Range (kPa) Reference

PANi/PDMS 0.641 200 150 0.05–60 Zheng et al. 2020 [52]

PANi/Lignin/Acrylate 0.012 500 ± 200 500 ± 200 0–10 Arias-Ferreiro et al. 2022 [53]
Cracked-PANI foam/PDMS 0.0027–––0.055 60 90 0–5 Zheng et al. 2019 [54]
Ni@Cu/PANi/CF 0.0053–––0.011 30 70 0–180 Chen et al. 2022 [55]
PANi/Cellulose 1 – 2.23 70 100 2–90 Kannichankandy et al. 2021 [56]
Cellulose/PANi (RFP3) 0.008 – 4.91 129 145 0–12.5 This work

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G. Ferreira et al. Chemical Engineering Journal 480 (2024) 147995

Fig. 7. (a) and (b) Repetition cycle for pressure sensor device under 1.23 (Blue) and 5 kPa (Red), respectively; Each graph has been magnified for two different cycle
ranges (one close to 100 cycles and another around 800 cycles) that are adhered to their corresponding curves (below) with relative assigned colors; (c) Weight
identification system incorporated with ESP32; (Supplementary Video 1). (d) Schematic of Smart IoT pressure sensor design application with IoT connected server to
communicate pressure sensor data; and Snapshots from the working locking-system, LED blinks, when correct code is inserted (Supplementary Video 2).

and another around 800 cycles) for each data are presented to have a
close look at the output signals of the cycles. During the entire experi­
ment, a high stability of the device performance can be observed as
shown in Fig. 7(a) and (b), which supports the sample as a potential
candidate for pressure sensing.
Furthermore, with several validation cycles it was possible to cali­
brate an ESP32 to be able to differentiate between the available weights.
The ESP32 is a microprocessor unit with an incorporated wireless block.
This module has in its structure several analog-to-digital converters
(ADC) that gather the data of the voltage variance at the terminals of the
pressure sensor, as well as provide the necessary feeding (5 V) to the
prototype. The ESP32 is programmed with Arduino IDE software. The
voltage variances will help identifying the weight placed on top of the
pressure sensor. The ESP32 will create an Asynchronous Webserver and
send data strings to a specific online directory. This address is accessed
on the computer through an internet browser. The data collected by the
computer is then translated to the amount of pressure being applied. A
supplementary Python programming was designed to command the
computer to access the data sent by the ESP32 and open an image-type
file corresponding to the weight placed on top of the pressure sensor, as
shown in Fig. 7 (c).
3.5. Self-powered sensor for secure keypad
Furthermore, the practical implementation of a sensor array was
built on advanced self-powered pressure sensing technology which has
been shown in Fig. 7(d). Corresponding supporting video has been
shown in Supplementary Video 2. The circuit diagram features nine
sensors, integrated with ADC and microcontroller distinguished by their
unique design that enables autonomous signal generation upon pres­
sure. Utilizing an ADC, the microcontroller reads signals generated by
each sensor upon touch/pressure. The programming logic is designed to
discern pressures exceeding a predefined threshold, ensuring precise
signal detection and interpretation.
The application revolves around the development of a secure keypad
system. Users interact with the sensors to input a four-pressure
sequence, creating a unique numeric pattern. The microcontroller in­
terprets and matches this pattern against a pre-stored database on the
cloud (server), forming the core of a secure access control mechanism.
Upon a successful match between the input pattern and the pre-
stored database, access is granted. A LED indicator blinks continu­
ously, visually confirming positive authentication. Conversely, an
invalid attempt does not trigger the LED indicator, accompanied by an
error message, signalling the failure to match the input pattern and
preventing unauthorized access. Extensive testing of the self-powered
keypad system reveals consistent and reliable performance. The self-
powered pressure sensors consistently generate signals upon touch,
and the microcontroller accurately processes and authenticates input
patterns. This reliability underscores the robustness of the system in
real-world applications. The application of these sensors in a secure
keypad system offers a practical and efficient solution for access control.
The seamless integration of these sensors with a microcontroller pro­
vides a sustainable and versatile platform for secure authentication. This
work not only demonstrates the viability of the proposed system but also
emphasizes its potential for broader applications within the realm of
self-powered sensor technologies.

11
G. Ferreira et al.
4. Conclusions
This study presents a novel approach to utilize recycled newspaper to
develop energy harvesting and pressure sensor devices. Various chem­
icals were utilized to modify the morphology of the samples. The addi­
tion of NaCl improved the density and distribution of the cellulose fibers,
leading to the production of more homogeneous samples. Subsequently,
the recycled newspaper samples were functionalized with PANi to
enhance conductivity and charge generation properties on the cellulose-
based substrate. An ecological energy device was constructed using the
functionalized sample as active layer and a silver metallic electrode
printed on Whatman paper. Notably, this device was developed entirely
from 100 % recycled paper without additional cellulose pulp and
without using any costly or harsh reagents or techniques. The devices
exhibited satisfactory performance in voltage and current outputs, with
the RFP3 device demonstrating the highest performance, achieving a
maximum current density of 33 mA m− 2 and power density of 0.35 W
m− 2. The energy harvesting capabilities of these devices can be attrib­
uted to the compression of PANi functionalized fibers, leading to an
increase in electronic density and subsequent charge transfer to the
collector layer. These devices were successfully utilized to illuminate a
series of several blue LEDs directly. Adding to its multifunctionality,
current functionalized papers were also identified as promising for
pressure sensing. The sensor devices developed during this study
demonstrated a fast response time (ranging from 129 to 145 ms), good
data reproducibility with over 2000 cycles of testing, and the ability to
differentiate pressure within a range of 12.25 kPa to 0.0025 kPa. The
designed pressure sensors exhibited a sensitivity of 4.91 kPa− 1 at low
pressure levels. An Internet of Things (IoT) pressure sensor application
was also developed, incorporating a wireless communication system.
Overall, this study presents promising results using 100 % recycled
newspaper as a sustainable and cost-effective material for sensor design
in smart packaging applications.
CRediT authorship contribution statement
Guilherme Ferreira: Conceptualization, Data curation, Formal
analysis, Methodology, Validation, Visualization, Writing – original
draft, Writing – review & editing. Shubham Das: Conceptualization,
Data curation, Validation, Visualization, Writing – original draft,
Writing – review & editing. Alberto Rego: Conceptualization, Data
curation, Formal analysis, Methodology, Validation, Visualization,
Writing – original draft, Writing – review & editing. Rafael R.A. Silva: .
Diana Gaspar: . Sumita Goswami: . Rui N. Pereira: . Elvira For­
tunato: . Luís Pereira: . Rodrigo Martins: . Suman Nandy: .
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgements
We acknowledge the project BRIGHT (Project reference: M-ERA-
NET3/0004/2021). This work was also partially financed by FEDER
funds through the COMPETE 2020 Programme and National funds from
FCT - Fundação para a Ciência e a Tecnologia, I.P., in the scope of the
projects LA/P/0037/2020, UIDP/50025/2020 and UIDB/50025/2020
of the Associate Laboratory Institute of Nanostructures, Nanomodelling
and Nanofabrication – i3N. G.F. also acknowledge the support from the
i3N- FCT – Portuguese Foundation for Science and Technology through
12
Chemical Engineering Journal 480 (2024) 147995
the Ph.D. (Scholarship grant no. UI/BD/151288/2021). This work was
also partially supported by European Union’s Horizon 2020 Research
and Innovation Programme under Grant Agreements number 952169
(SYNERGY, H2020-WIDESPREAD-2020-5, CSA) and 101008701
(EMERGE, H2020-INFRAIA-2020-1), and 101070255 (REFORM,
HORIZON-CL4-2021-DIGITAL-EMERGING-01). Partly of this work was
also supported by LISBOA-05-3559-FSE-000007 and CENTRO-04-3559-
FSE-000094 operations, co-funded by the Lisboa 2020, Centro 2020
programme, Portugal 2020, European Union, through the European
Social Fund, as well as by Fundação para a Ciência e Tecnologia (FCT)
and Agência Nacional de Inovação (ANI).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.cej.2023.147995.
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