Waste Management 123 (2021) 23–32

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Waste Management
journal homepage: www.elsevier.com/locate/wasman

Sustainable green strategy for recovery of glucose from end-of-life euro

banknotes
Samy Yousef a,c,⇑, Neringa Kuliešienė b, Sandra Sakalauskaitė b, Tomas Nenartavičius b,
Rimantas Daugelavičius b
a
Department of Production Engineering, Faculty of Mechanical Engineering and Design, Kaunas University of Technology, LT-51424 Kaunas, Lithuania
b
Department of Biochemistry, Vytautas Magnus University, Kaunas, Lithuania
c
Department of Materials Science, South Ural State University, Lenin Prospect 76, 454080 Chelyabinsk, Russia

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

Article history: Usually, Euro banknotes are made from cotton substrates and their waste is disposed of in landfill or is
Received 1 March 2020 incinerated. In order to valorize the end-of-life euro banknotes (ELEBs), the substrates were used in this
Revised 18 June 2020 research for cellulase production via submerged fungal fermentation (SFF), and the resultant fungal cel-
Accepted 7 January 2021
lulase w s used in ELEBs hydrolysis process for extraction of glucose. The experiments were started by
Available online 4 February 2021
exposing the ELEBs to different types of pretreatments, including milling process, alkali (NaOH/urea solu-
tion), and acid leaching to remove any contamination (e.g. dyes) and to decrease the crystallinity of cel-
Keywords:
lulose (the main element in cotton substrate) thus increasing the degradation rate during the
End-of-life banknotes
Cellulase
fermentation process. The effect of pretreatments on the morphology and chemical composition of
Hydrolysis ELEBs was observed using Scanning Electron Microscope and Energy Dispersive Spectrometry.
Fermentation Afterwards, Trichoderma reesei-DSM76 was used for cellulase production from the treated ELEBs with
Circular economy high cellulase activity (12.97 FPU/g). The resultant cellulase was upscaled in a bioreactor and used in
Glucose ELEBs hydrolysis. Finally, the results showed that the optimized pretreatment methods (milling followed
by leaching process) significantly improved the cellulase activity and glucose recovery, which was esti-
mated by 96%. According to the obtained results, the developed strategy has a great potential for conver-
sion of ELEBs into a glucose product that could be used in biofuels and bioplastics applications.
Ó 2021 Elsevier Ltd. All rights reserved.

1. Introduction
In 1999, euro was introduced for the first time to world finan-
cial markets as an accounting currency instead of former European
currencies. Subsequently, in 2002, euro coins and banknotes
entered circulation as a daily operating currency of the original
EU Member States. Subsequently, euro quickly took over the for-
mer national currencies and expanded throughout the European
Union to circulate in the majority of the EU countries during the
period 2002–2015 and Lithuania was the last to circulate euro
(Commission, 2006, Guedes et al., 2013, Troiano et al., 2017).
Now, euro has become the second-largest reserve currency and
the second-most traded currency in the world after the United
States dollar. The substrates of euro banknotes are usually made
of cotton paper fitted inside the magnet (for reading by ATMs)
and nylon bar for visual inspection (holographic security thread)
and these features are common in all euro banknote series as
⇑ Corresponding author.
E-mail address: ahmed.saed@ktu.lt (S. Yousef).
shown in Fig. (S1) (Sonnex et al., 2014). In 2017, some series were
made from multi-layer polymers due to economic and safety con-
siderations (Abdelshafi et al., 2017), but it has not been generalized
to all the categories so far and cotton is still predominant in the
majority of substrates categories (Griffin et al., 2018). The average
lifespan of a banknote is 3 years; then it may be disposed of by two
different techniques based on the type of substrate. With regard to
polymer-based banknotes, the end-of-life waste is crushed, then
turned into small granules that can be used as secondary materials
to produce some plastic products of suitable quality, while cotton-
based waste is usually disposed of by burning and incineration
(Luján-Ornelas et al. 2018, Worrell, 2014).
Unfortunately, there is no specific value for annually generated
end-of-life euro banknotes (ELEBs), where these values need to be
approved by the Governing Council of the ECB, which is not
allowed at the moment. However, these values can be estimated
based on the statistical data of the value of euro banknotes pro-
duced in 2019, which was estimated by 113.2 billion euros). The
average weight of this amount of euro banknotes can be estimated
by 57 tons (assuming that 20 euro is the main series) and 120 tons

https://doi.org/10.1016/j.wasman.2021.01.007
0956-053X/Ó 2021 Elsevier Ltd. All rights reserved.
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
(assuming that 10 euro is the main series). This amount is gener-
ated from the EU zone only (445 million people), which means that
the total amount of generated banknotes waste globally is equal
more than 10 times this value. These estimated values indicate that
banknotes in general produce a huge amount of waste that has not
been considered until now. This type of waste can be classified as
cotton-based waste and this type of waste contains nitrogen (N)
and sulphur (S) that can emit some toxic NOx and SO2 during
the treatment, by incineration, and thus causing some serious envi-
ronmental problems (Yousef et al., 2020).
In order to maximize the benefit of this waste, our team has
developed an integrated approach to recover cotton and other ele-
ments using different chemical processes (Yousef et al., 2019a).
However, the main challenge for industrial application is the safety
element, as this technology gives sensitive and accurate informa-
tion to the public, which increases fraud and supply. In order to
maintain the safety factor, our team has exploited the presence
of cotton heavily and turned it into high-value materials using
the pyrolysis treatment in a reactor with a capacity of 300 g
(Yousef et al., 2020). Although our team has succeeded in convert-
ing this waste into 40% fuel and 50% biogas, incineration, pyrolysis,
and gasification processes have some reservations related to con-
sumed energy and emissions during the reaction process. There
are also other restrictions related to energy consumption (up to
900 °C), chemicals and reagents during the conversion process
used to obtain oil, gas, and char (Rodriguez et al., 2018, Dong
et al., 2018, Alvarez et al., 2019). In addition, the obtained energy
products are usually contaminated by many other gases (like
CO2, N2, etc.) what needs another process to separate these gases
using amino technology (Yousef et al., 2019b, Zhou et al., 2017,
Rafiee et al., 2017), which is classified as attractive chemical pro-
cess for CO2 capture via hydrate formation because of its ability
to mix with water through hydrogen bonding and because of its
nontoxic nature, nonvolatility, and eco-friendliness (Pandey et al.,
2020). Therefore, the choice of a disposal method of banknote
waste is constrained by a security factor (especially, chemical
structures and components), economic benefit, whereas the envi-
ronmental issue is considered to be the main challenge for stake-
holders interested in this field.
Since cellulose is the main component of banknote waste with a
huge amount of cellulose-rich material with high degree of poly-
merization and crystallinity microfiber bundles with glucan in
the range 0.81–0.95 (Mohammadi Amirabad et al., 2018; Yousef,
2019a), which leads to possible classification of banknote waste
as Lignocellulosic waste substrates (they have a high carbohydrate
content), energy conversion solutions could become potentially
serious solutions for production of high added-value energy pro-
duct (biofuels and chemicals) and achievement of circular econ-
omy and renewable energy concept at the same time (Ge et al.,
2018). Biorefinery or bioprocesses could be another potential envi-
ronmental solution to produce high added-value energy product
(biofuels and chemicals) (Sarsaiya et al., 2019, Kan et al., 2017).
An especially big number of studies have been developed to inves-
tigate intensively fossil fuels used as an alternative renewable
source and the results showed that this approach could be a major
contributor to the future energy supply (Gottumukkala et al.,
2017). In most of the cases of bioprocesses utilizing cotton waste,
enzymatic hydrolysis are needed for conversion of cellulose to fer-
mentable sugars (Bhowmick et al., 2018, Hassan et al., 2019, Marín
et al., 2019). However, cotton-based waste, including banknote
waste, contains a highly compact and crystalline structure of cot-
ton, resulting in a very low bioconversion rate and yield due to
the recalcitrant nature of lignocelluloses (Solarte-Toro et al.,
2019). Also, it was noted in the studies that dealt with this waste
and its biological treatments that the presence of the contaminated
elements (like inks and dyes) and residual components in the feed-
24
Waste Management 123 (2021) 23–32
stock is one of the main challenges that need to be overcome. The
presence of these elements represents a major impediment for
microorganisms to break the metallic and chemical bonds between
ink pigments, then reaching to cellulose layers and achieving full
degradation (Hasanzadeh et al., 2018). In order to have an effective
hydrolysis process and to improve the digestibility of cotton-based
waste, polymers of cellulose and hemicelluloses should be released
the first from fibrils during ‘‘pretreatment”, while general ideas of
various pretreatment technologies should be to alter or remove lig-
nin and hemicelluloses, and thus to increase surface area and to
decrease crystallinity of cellulose (Quartinello et al., 2018, Dimos
et al., 2019).
In the literature, degradation of highly crystalline structure of
cellulose requires synergy of endoglucanases (EC 3.2.1.4), exoglu-
canases (EC 3.2.1.91) and b-glucosidases (EC 3.2.1.21) in a complete
cellulase system. However, the cost of enzyme remains one of the
main obstacles in the commercialization of these processes. It was
estimated that the cost of cellulase accounts for 10–40% of the total
production cost in the current biorefinery process (Mu et al., 2019,
Hasanzadeh et al., 2018). To avoid that, recently, microbial cellu-
lase production (with different microorganisms such as Aspergillus
niger, Trichoderma reesei, etc.) using cellulosic residues via sub-
merged fermentation and solid-state fermentation has been used
as low-cost and promising cellulase producing techniques in terms
of relatively low energy consumption and simple downstream pro-
cessing (Hu et al., 2018, Du et al., 2018, Taherzadeh-Ghahfarokhi
et al., 2019, Hasanin et al., 2019). With regard to these microorgan-
isms, Trichoderma reesei Simmons was selected for the present
research as a commercial product with high activity widely used
by cellulase producers (Taherzadeh-Ghahfarokhi et al., 2019,
Phwan et al., 2018, Hu et al., 2018). Also, end-of-life euro ban-
knotes (ELEBs) were exposed to mechanical and chemical pretreat-
ment (to decree their crystallinity) followed by fermentation and
hydrolysis processes for glucose recovery using benchtop
fermentor.
2. Experimental
2.1. Banknote waste, microorganism, and chemicals
End-of-life euro banknotes (ELEBs) in the form of small pieces
(size of approximately 2
10 mm) were collected from municipal
solid waste landfill. Fourier-transform infrared spectroscopy (FTIR)
was used to determine chemical structure and base element in the
received ELEBs. Based on the FTIR analysis (which is explained in
the section of results and discussion), the supplied ELEBs were
made from cotton. Trichoderma microorganism was purchased
from DSMZ, Germany (Leibniz-Institut DSMZ - Deutsche Samm-
lung von Mikroorganismen und Zellkulturen GmbH). All other
chemicals, including NHO3, NaOH, etc., were purchased from
Sigma-Aldrich.
2.2. Design of the new bio-recycling strategy
The layout of the developed strategy was designed on the basis
of the already present bioconversion technologies; in particular
waste pretreatment, fermentation media, and Hydrolysis process
(Wang et al., 2018). Fig. 1 shows the layout of bioconversion strat-
egy developed in the present research. The strategy is composed of
four stages: I) preparation of the spore suspension, II) cultivation
process, III) euro banknote waste pretreatment (using milling
and chemical treatment), V) shake fermentation process (lab scale),
and IV) pilot fermentation and hydrolysis processes for glucose
recovery using benchtop bioreactor. All these steps, including the
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
Fig. 1. The layout of the developed bioconversion strategy.
optimum conditions, are explained in detail in the following
sections.
2.2.1. Preparation of the seed culture suspension
The layout was started with preparation of spore suspension by
dispersing 10 ml of Trichoderma microorganism on the surface of
20 ml of potato dextrose agar (PDA) in a petri dish
(90 mm
15 mm), followed by incubation at 27 °C for 7 days.
The resultant seed culture was extracted as a suspension (wet con-
centrated seed culture) after having mixed it with 10 ml of deion-
ized water. After that, Hemocytometer was used to determine the
spore concentration in the obtained suspension, which was esti-
mated by 3
107 spores/ml (Fig. 1I). Finally, the obtained seed cul-
ture suspension was exposed to centrifugal treatment at 3000g for
10 min., followed by a filtration process (using a 0.22 lm mem-
brane filter) to prepare the concentrated seed culture solution
(CSCS).
2.2.2. Cultivation of the seed culture suspension
Mandel’s medium containing 20% (w/v) glucose was used as a
cultivation medium. The medium was composed of (g/l): urea,
0.3; KH2PO4, 2; (NH4)2SO4, 1.4; MgSO4, 0.3; CaCl2, 0.4; FeSO4,
0.005; MnSO4, 0.0016; ZnSO4; 0.0014; CoCl2, 0.002. Since the selec-
tion of nitrogen source (or inducer in fermentation medium) has a
significant effect on the cellulase production, therefore, the initial
experiments were conducted using five different nitrogen sources,
including Soybean meal, NH4NO3, Peptone, Urea, and a mixture of
them (beef extract, (NH4)2SO4, yeast extract, peptone, NaNO3, urea
and soybean meal) (Mandels et al., 1969). Then the optimal variant
was selected based on the highest cellulase activity. In order to
prepare a high concentration spore solution (HCSS), 10 ml of CSCS
with concentration of 200 spores/ml were inoculated into 100 ml
of the prepared mineral solution (pH 6.3–6.5) at 27 °C for
25
Waste Management 123 (2021) 23–32
10 min., and then shaken at 150 rpm up to 48 h. to prepare the seed
culture medium (Fig. 1II).
2.2.3. Banknote waste handling and pretreatment
Generally, pretreatment of the feedstock is one of the key player
controlling quality and yield of the final product (Dong et al., 2019,
Ashraf et al., 2018). Also, it has been proposed to ease enzyme
access to cellulosic fiber and to decrease crystallinity. Alkali
(NaOH/urea solution) pre-treatment is widely used for this pur-
pose after having crushed the biomass (banknote in the present
case) to small pieces (Bian et al., 2019). Since ELEBs were collected
from municipal solid waste landfill in the form of small pieces, raw
ELEBs were exposed directly to alkali (NaOH/urea solution) pre-
treatment without any additional crushing. However, it was hard
to decompose ELEBs of such size. Therefore, the raw samples were
milled to fine powder on a micro scale with uniform size that led to
degrade all particles at the same time during the fermentation pro-
cess, then treated using two types of chemical treatments: alkali
and leaching treatment to remove heavy metals from the dyes in
order to decrease crystallinity (Fig. 1III). In case of alkali, the waste
was soaked in a mixture of 12% NaOH (w/v) and 7% urea (w/v), and
then stored at 20 °C for 6 h. Later, these samples were thawed
and washed with DI water until pH dropped to 7.0 (Wang et al.,
2018). Since intaglio inks are widely used in banknote printing
and these types of inks are composed of metallic pigments and
organic fraction joined together using chemical and mechanical
bonds, thus, the leaching process was used as another chemical
pretreatment to solubilize metallic pigments from ELEBs under
the effect of sound waves. The leaching experiments using Nitric
acid (concentration 60%) were conducted based on the optimum
leaching conditions obtained by (Yousef et al., 2019b), particularly
2 M HNO3 at 70 °C for 10 min. The leaching process was followed
by a float-sink separation process (separation by density in water
medium) for removal of any remaining organic substances of ink
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
layers and floating of polymer strips on the water surface, thus lib-
erating and purifying the cotton substrate from any contaminated
elements. Fig. (S2) shows images of the untreated and treated
ELEBs samples. The samples are denoted as ELEB0 to ELEB3 based
on the type of pretreatment as illustrated in the Table 1.
2.2.4. Fermentation process
According to the concept of Technology Readiness levels (TRL),
the experiments of any new technology (including biological pro-
cesses) should be passed through two main phases: a laboratory
phase to obtain the optimal conditions (e.g. nitrogen source, cellu-
lase activity, etc.) and an upscaling phase to simulate and study the
effect of upscaling on the yield and quality of the final product pre-
cisely (Baron et al., 2019). Also, the upscaling phase is very impor-
tant for the business sector and decision-makers, as this
technology is promoted and applied on an industrial scale. Within
TRLs, fungal cellulase was produced on untreated or treated ELEBs
via a submerged fermentation process in two phases. The first
phase (lab scale experiments) was employed to determine the
optimum conditions of the fermentation process, including nitro-
gen source. The experiments were carried out in a glass flask of
100 ml capacity in a laboratory shaker incubator at 27 °C and
200 rpm for 12 days with inoculation size of 10 g/l (ELEBs/HCSS)
(Fig. 1IV). While, the second phase focused on simulation of the
fermentation process at industrial scale. The upscaling fermenta-
tion experiments were performed according to the optimum con-
ditions obtained from the first phase (in particular at 27 °C and
200 rpm in compressed air). The upscaling experiments were car-
ried out in a 3-L benchtop fermentor (Fermac 360, Electrolab, UK)
and the main components are shown in Fig. 1V. The pilot fermen-
tation experiments were performed without the intervention of
oxygen to avoid the potential complexity of fermentation reaction.
2.2.5. Analysis of cellulase activity and hydrolysis of ELEBs
The effect of different pretreatments and nitrogen sources on
the total cellulase activity was studied by filter paper activity
(FPase) standard method and can be calculated using Eq. (1)
(Adney et al., 1996).
FPase activity ðFPU=mLÞ ¼
0:37
Concentration of enzyme that release 2:0mg glucose
ð1Þ
The fungal cellulase received from pretreated and untreated
ELEBs was filtrated by the end of fermentation process and used
as a substrate for hydrolysis process and production of glucose.
The hydrolysis experiment was conducted on the untreated and
treated samples at 50 °C and 300 rpm for 382 h (16 days). Usually,
sterilization process (such as UV irradiation, chemical process,
addition of antibiotics, etc.) is applied during enzymatic hydrolysis
of biomass to avoid the growth of unwanted bacteria. However,
such treatment is expensive and can modify the chemical structure
of the feedstock, which makes the hydrolysis mechanism more
complex. Therefore, classical sterilization in a regular oven was
used in the present research (as an economic process) to sterile
the purified cotton substrate (before starting fermentation and
hydrolysis process) at 70 °C for 30 min at ambient pressure. This
helped to safeguard complete purification and sterility of the sub-
strates (Wu and Cheng, 2005). In order to study the effect of the
Table 1
ELEBs sample codes.
As received small pieces (ELEBs) Type of the applied pretreatment
– –
Milling
Milling
Milling
26
Waste Management 123 (2021) 23–32
hydrolysis time on glucose yield, the samples were taken at regular
time intervals every 24 h and the hydrolysis yield was determined
using Eq. (2) (Hu et al., 2018). Finally, the yield of the formed glu-
cose was analyzed by ultra-performance liquid chromatography
(HPLC, Waters, UK).
Amount of glusco released ðgÞ
Hydrolysis yield ðFPU=mLÞ ¼
Amount of intial cellouse in substrat ðgÞx 1:111
ð2Þ
3. Results and discussion
3.1. Analysis of the untreated and treated banknote samples
3.1.1. Chemical analysis of the ELEB substrate
As mentioned in the introduction section, the banknotes are
composed of a substrate covered by ink layer and some compo-
nents (e.g. holographic security thread and magnetic thread) that
make it hard to determine chemical structure of the substrate.
Also, the FTIR performed directly on the supplied banknotes would
show an inaccurate analysis as a result of overlapping of function
groups of FTIR. In order to avoid the aforementioned problems,
FTIR was performed on ELEB3 (without dyes and other compo-
nents). Fig. (S3) shows FTIR spectra of the treated ELEB sample.
As shown in FTIR analysis, the treated substrate has several peaks,
i.e. O–H stretch, CH bend and C–O stretching vibrations at
3410 cm1, 2918 cm1 and 1045 cm1, respectively. Also, O–H
bending vibration of absorbed water was detected at 1749 cm1.
Another absorbance vibrational band was noted at 1156 cm1
(C–O–C Stretch) associated with cellulose I and cellulose II. The
presence of these groups confirms that the supplied ELEB sub-
strates were made from pure cotton (Hafrén et al., 2005, Gaspar
et al., 2014).
3.1.2. Observation of the pretreatment mechanism
Optical color microscope was used to inspect the outer surface
of the untreated samples and to observe the treatment mechanism.
Fig. 2(A–E) shows the metallographic images of the supplied ELEB0
sample (untreated) with a scale of 500 lm. As shown in the photos,
the supplied sample in the form of small pieces had several distin-
guishing features, including (dark and light) intaglio printed
images (saturated by various inks with different colors) and bright
parts representing holographic security thread. Once the ELEB0
sample was exposed to milling pre-treatment, all these features
mixed together and the holographic security thread started to sep-
arate in the form of small pieces of polymer films as a result of
shear stress resulted during the milling process Fig. 3F, G, which
was more than enough to overcome the friction bonding between
holographic security thread and ELEBs substrate. Under the effect
of sound wave supported by leaching process (ELEB3), most of
the pigments were removed as a breakage of Van-der Waals forces,
covalent bonding, and polar interactions between dyes, substrate
and cellulose, thus liberating the magnetic bars as shown in
Fig. 2H, I. In case of the sample treated (ELEB2) by alkali, the fea-
ture didn’t change too much compared with ELEB1. Finally, after
having applied the float and sink treatment (separation by density)
followed by milling process, all polymeric components were
Sample code
– ELEB0
– – ELEB1
Alkali Float and sink ELEB2
Leaching Float and sink ELEB3
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
Fig. 2. Metallographic images of the untreated and treated end-of-life euro banknotes.
Fig. 3. SEM-Mapping analysis of the untreated and treated end-of-life euro banknotes.
removed completely, thus obtaining pure cellulose powder as
shown in Fig. 2J.
3.1.3. Morphology and chemical analysis of the supplied materials
In order to check the morphology and chemical composition of
the banknote samples before and after different pretreatments,
Scanning Electron Microscope (SEM) and Energy Dispersive Spec-
trometry (EDS) were used. Fig. 3A–D shows the SEM photos of
ELEB0, ELEB1, ELEB2, and ELEB3, respectively. As shown in
Fig. 3A, cotton fibers had a complex coress-link with high crys-
tallinity and these structures did not change after treatment by
alkali, Fig. 3B. Once the milling process had been applied on the
samples, the fiber was liberated significantly Fig. 3C. Finally, after
applying the leaching treatment, the fiber was separated com-
pletely and had clear surface.Fig. 3D. Fig. 3E–H shows SEM-
Mapping analysis of ELEB0, ELEB1, ELEB2, and ELEB3, respectively.
As shown in the resulted mapping analysis, the surfaces of ELEB0,
ELEB1, and ELEB2 were contaminated by multiple metals, includ-
ing such elements as Mg, Al, Fe, Ca, Si, etc. It means that alkali
treatment doesn’t affect the ink layer Fig. 3G, while most of these
27
Waste Management 123 (2021) 23–32
elements were removed after the leaching process Fig. 3H
(Yousef et al., 2019a, Gaspar et al., 2014).
3.2. Observation of fungal growth
The cellulase production using Trichoderma reesei microorgan-
isms is changed independently of the experimental setup, includ-
ing cultivations, inducer, etc. Also, the changes in
micromorphology can be related to the protein concentration inde-
pendent of the strain used (Novy et al., 2016). Therefore, optical
microscope was used to observe the fungal growth on the potato
substrate after 2, 4, and 6 days (under the same conditions listed
above). Fig. (S4A-C) shows the morphology of the fungi growth
on the potato substance after 2, 4, and 6 days, respectively. As
shown in the photos, distinct micromorphological differences were
revealed between strains after a few days. The fungal hyphae and
spores could be observed from the second and the fourth day,
respectively. It was noted that very small green dots started to
appear after 2 days on the white fungi layer, then these dots were
growing gradually over 4 days followed by significant growth after
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
6 days and the substrate became coated with green thin film,
which resulted in an increased degree of branching in submerged
cultures of fungus. In order to confirm the results described above
and to check on the structure of the obtained fungus, the prepared
suspended solution was observed. Fig. (S4D) shows the structure of
the collected fungi in the form of suspension after 7 days. As shown
in the Fig, filamentous fungus is the main component in the growth
and presence of these features means that the fungi were grown
successfully in the ideal conditions (Li et al., 2016).
3.3. Observation of the bio-decomposition of ELEBs during the
fermentation process
Based on FTIR results, cellulose was the main element in the
supplied ELEB, so a high yield of glucose could be expected, espe-
cially if other components, such as lignin and hemicelluloses were
not observed. However, this goal could not be achieved because of
two major factors, high crystallinity of cellulose and ink layer,
which led to delay of decomposition of the ELEB samples. Also,
these factors prevented growth and penetration of fungi on the
surface of the ELEB substrate. That’s why the pretreatment was
used as mentioned before. SEM was used to check the effect of dif-
ferent pretreatment on the decomposition of ELEBs, including their
morphology and their degradation mechanisms in the course of
different cultivation periods. The SEM observation process was
performed on the treated and original ELEB samples. The process
started by picking up the examined ELEB samples (10 ml) from
the cultivation media after 1, 3, 5, and 7 days using Single-
Channel Pipettor; then they were filtered and left overnight at
35 °C for complete drying. Fig. 4 shows the surface morphology
Fig. 4. Morphology of the decomposed samples A–D) ELEB0, E–H) ELEB1, I–L) ELEB2, and M–P) ELEB3.
28
Waste Management 123 (2021) 23–32
of the dried ELEB0- ELEB3 samples. It seems that morphology
and decomposition of ELEB0 were not affected significantly by
the formation process. The cultivation process even increased as
a result of its high crystallinity (Fig. 4A–D).
After exposing the supplied banknote to grinding pretreat-
ment (ELEB1), after the first day several cracks started to appear
in the organic components in the dye layer under the effect of
shaking force (Fig. 4E). On the third day, the fungi started to pen-
etrate into the ELEB1 substrate through the established cracks
and break the chemical and mechanical bonds between the dye
layer and main component of the substrate (cellulose), which
led to separation of the dye layer, including pigment components
(Fig. 4F). On the fifth day, the fiber in the cellulose substrate
became bare and started to decompose to small molecules in
the form of cellulose nanocrystal precursor (Fig. 4G). It was noted
that decomposition was performed layer by layer (exfoliation
process) in this batch, because cotton is composed of high crys-
tallinity microfiber bundles (Fig. 4H). The decomposition mecha-
nism of ELEB2 was faster than that of ELEB1 due to their stronger
surface contact with the media, which led to acceleration of the
reaction between the milled substrate and fermentation media
(Fig. 4I–L). In case of the last sample (ELEB3), it was easier to
decompose cellulose than other samples since there were no
dyes and contamination on the fiber surface, resulting breakage
of the hydrogen bonds in crystalline regions of cellulose
(Fig. 4M–O). Also, it was noted that by the end of the fermenta-
tion process, some residual particles were produced (Fine fiber
particles) as a result of decomposition of cellulose into different
products (e.g. d-glucose, levoglucosan, glucopyranose, etc.)
(Fig. 4P) (Reddy et al., 2016).
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al. Waste Management 123 (2021) 23–32

3.4. Selection of optimum conditions for the fermentation process agro-industrial residues (5.6 FPU/g), and lignocellulosic (2.9 FPU/
g), which can contribute to increase in bioconversion rate. Despite
This section focuses on selection of optimum conditions for the the promising results, the activity of cellulase produced from ban-
fermentation process, including pretreatment and constraining of knotes is still lower than that found in horticulture waste (15 FPU/
nitrogen source in order to achieve maximum cellulase production. g) and textile waste (18.75 FPU/g). This moderate decrease in cel-
Fig. 5A demonstrates the results of cellulase production till 12 days lulose production is due to three main reasons: different composi-
using ELEB0, ELEB1, ELEB2, and ELEB3 samples as a fermentation tion of the feedstock, use of different types of pre-treatments and
substrate in presence of sole nitrogen source (Mandel’s medium microorganisms during the biological processes. It should be men-
nitrogen source; a mixture of yeast extract, urea and (NH4)2SO4) tioned that the selection of the optimum pretreatment and
(Mandels et al., 1957). As shown in the figure, the original sample microorganisms constrained by maximum cellulase production is
was not suitable for growing fungi on its surface because of three still under construction by our research group (Hu et al., 2018).
reasons; dyes, high crystallinity of cellulose, and usually these
types of waste are contaminated by different types of drug (e.g. 3.5. Pilot scale fermentation process
Cocaine, Bacteria, etc.) during the currency trading (Armenta
et al., 2008, Jenkins et al., 2001), which leads to stopped growing The untreated and pretreated banknotes were fermented by
of fungi and killing most of them. In case of ELEB1 sample, the fer- fungi in 3 L bioreactor to study the effect of upscaling of fungal fer-
mentation process started slowly, so the contact surface between mentation on the cellulase production and fermentation time. The
the fermentation media and substrate was increased and its crys- pilot fermentation experiments were performed according to the
tallinity was reduced a little by milling (Bian et al., 2019), but still optimum results obtained from Section 3.4, particularly using
the dyes and toxic materials remained on the surface. With regard Mandel’s mixture source with the highest cellulase activity
to the sample treated by alkali (ELEB2), most of toxic materials (12.62 FPU/g) as an optimum nitrogen source. During the pilot
were removed and the substrate of ELEB2 sample turned into suit- experiments, rapid fungal growth was noted on the surface of ELEB
able ambient to grow fungi; however, presence of dyes prevented samples in the form of white hyphens with less fermentation time
penetration. (~4 days with reduction 25% compared with lap scale fermentation
This problem could be overcome by leaching process when experiments). In addition, the cellulase activity of ELEB3 and ELEB2
most of pigments are removed from ELEB3, thus increasing the cel- was not affected too much by upscaling; it improved only by ~3%,
lulase activity from 11.34 FU/g (ELEB2) to 12.62 (ELEB3) FPU/g because these samples had uniform substrate size and chemical
with improvable offing ~12%. These results confirm the SEM obser- composition, thus leading to uniform decomposition of substrates,
vation. Therefore, milling pretreatment followed by leaching pro- especially in case of ELEB3. Also, after chemical treatments, the
cess was selected as an optimum pretreatment. In order to select banknotes waste became more accessible to fungal growth and
the optimum nitrogen source, in addition to Mandel’s medium- metabolism, thus increasing the cellulase activities with the same
mixture as a nitrogen source, other four nitrogen sources were rate at lab and pilot scale (Singhania et al., 2017). While the cellu-
used to study the effect of nitrogen source on cellulase production. lase production in case of ELEB0 was increased significantly by
Since ELEB3 sample manifested the highest cellulase activity (as ~20%, see Fig. 6. This improvement in case of ELEB0 sample is a
shown in the previous section), the experiments were performed result of manifold and changing in the fungal morphology, which
on this sample. Fig. 5B shows the effect of nitrogen sources on provided higher contact area and better oxygen transfer, thus con-
the cellulase activity of ELEB3 sample. As shown in the figure, tributing to the enhanced fungal growth and metabolism (Hardy
the use of Mandel’s medium-mixture as nitrogen source resulted et al., 2017).
in the highest cellulase activity of 12.62 FPU/g, and soybean meal
resulted in the second highest cellulase activity of 11.16 FPU/g 3.6. Enzymatic hydrolysis of ELEBs
(with reduction 13%), while peptone and urea manifested the low-
est cellulase activity estimated by 2.03 FPU/g and 1.93 FPU/g, As mentioned in the introduction section, cellulose is the main
respectively. Therefore, Mandel’s medium was selected as an opti- component of ELEBs composed of parallel unbranched D-
mal nitrogen source among others sources with high cellulase pro- glucopyranose linked by b-1,4-glycosidic bonds. These units are
duction and these results agree with the results found in the joined by Van der Waals forces and hydrogen bonds, forming
literature (Phwan et al., 2018, Hu et al., 2018, Wang et al., 2018). highly organized microfibrils of high crystallinity. In addition,
It can be seen that banknote waste manifested an appreciable cel- some amorphous cellulose regions result when these bonds are
lulase activity (12.97 FPU/g), compared to activity of cellulase pro- broken. Amorphous cellulose is hydrolysed at a much faster rate
duced from that found in mild alkali-treated rice straw (11 FPU/g), than partially crystalline cellulose because of the lack of its

14 14
Cellulase activity (FPU/g)

Cellulase activity (FPU/g)

12 ELEB0 (A) 12 (B)

10 ELEB1 10

ELEB2 8
8
6
6 ELEB3
4
4
2
2 0
0 Mixture Soybean NH4NO3 Peptone Urea
0 1 2 3 4 5 6 7 8 9 10 11 12 meal
Fermentation time (days) Nitrogen source

Fig. 5. A) Cellulase activity achieved with untreated and treated ELEB samples till 12 days, B) Effect of nitrogen sources on cellulase production using Trichoderma.

29
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
Cellulase activity (FPU/g) 15
Lab experiments
12
Pilot experiments
9 indicated that a comparable enzymatic effect was obtained using
6 cotton-based waste hydrolysis (Darwesh et al., 2020). Also, this
3 tion of cellulose into different products and formulation of cellu-
0 results, one of the main challenges in glucose production from
ELEB0 ELEB1 ELEB2
Sample code
Fig. 6. Cellulase activity achieved with untreated and treated ELEB samples using
the bioreactor.
intramolecular arrangement. This facilitates its digestion in the
course of hydrolysis process and decomposition of carbohydrate
in cellulose into sugar molecules (e.g. sucrose being broken down
into glucose and fructose) (Mejias et al., 2018, Hasanzadeh et al.,
2018). The enzymatic hydrolysis process was employed to hydro-
lyze the cellulosic component (in the euro-banknotes waste) into
glucose product.
The resulted fungal cellulose was formed using upscale experi-
ments (Section 3.5) with total cellulase activity. ELEB0-ELEB3 sam-
ples of 0.64, 6.97, 11.52, and 12.97 FPU/g, respectively, were used
in the hydrolysis process. Fig. 7 shows the glucose yield as a func-
tion of hydrolysis time for all the ELEB samples for 16 days. It is
clear that the high crystallinity of ELEB0 sample impeded conver-
sion of its substrate into glucose. After decreasing its crystallinity
by milling process, more than 18% of ELEB1 sample were converted
to glucose. In case of ELEB2 and ELEB3 samples, it seems that the
chemical pretreatment using alkali and leaching process was suc-
cessful to convert more than 42% of substrates into glucose after
6 days in the first stage. It was achieved with the help of higher
ratio of endocellulase in fungal fermentation filtrate, which led to
quick breakdown of the crystalline structure of cellulose in both
samples, thus accelerating the rate of hydrolysis in the initial phase
(for 6 days) (Hardy et al., 2017). After this point (second phase), the
conversion rate of ELEB2 sample was growing slowly until it
reached 71% after 15 days as a result of cellulose sedimentation
in the form of mixture contaminated with some heavy metals
and dye pigments. This resulted in strong obstacle for hydrolysis
process.
100
80
Glucose yield (%)
60
40
20
0 by our research group in the present and previous studies and the
0 50 100 150 200 250
Hydrolysis time (hr.)
Fig. 7. End-of-life euro banknotes hydrolysis.
Waste Management 123 (2021) 23–32
On the contrary, ELEB3 sample was continuing its hydrolyzation
until conversion of more than 96% into glucose in less time
(13 days) as a result of removing most of the contamination (which
was mixed with waste) during the leaching process. These results
fungal cellulase, when compared to commercial cellulase in
means that only 4% were not converted as a result of decomposi-
lose nanocrystals (Fig. 4P) (Yousef et al., 2019a). As shown in the
ELEB3 ELEB is its highly compact and crystalline structure. Also, the
appropriate pretreatment can result in the cellulose crystallinity
reduction and help to improve digestibility of ELEB and to achieve
a high yield of glucose during the hydrolysis process when impuri-
ties, mercerization, and other contaminations are removed from
the feedstock. When pretreatment helps to transform cellulose I
(native form of cellulose with parallel cellulose chains in a unit
cell) to cellulose II (a regenerated form of cellulose with an antipar-
allel direction of cellulose chains in a unit cell), this may improve
anaerobic digestion of ELEB (Cavka et al., 2013, Hasanzadeh
et al., 2018). Overall, the results of the present research show the
possibility of using banknote waste as a substrate in submerged
cellulase production. Further efforts are required for optimization
of fermentation conditions and selection of fungi.
3.7. Contribution of this research to sustainability
Banknote industry is one of the most important and a critical
industry that consumes a huge amount of high-purity paper cot-
ton. Most of this cotton is lost by the end of the banknote’s life
in the form of municipal solid waste. The recycling of this cotton
in the form of high added-value products (glucose in the present
research) could be contributed essentially to sustainability of ban-
knote industry. However, this process should be constrained by
three factors: selection of green processes (without toxic materials
or using chemicals able to regenerate at the end of the reaction),
less input of energy, less gas emissions, and high economic benefit
(Hole et al., 2019). All of these were taken into account while
developing the strategy, where the fermentation process using
fungi is class a green promise technology (bio-recycling technol-
ogy) of biomass without generating a toxic material or gases was
compared with other conversion technologies (e.g. pyrolysis and
gasification, etc.) (Gupta et al., 2020). Also, pre-treatment using a
leaching process can be classified as a sustainable process, espe-
cially when some studies were developed to regenerate the spent
acid using high-efficiency membranes.
Since the banknote industry is classified as a critical industry
that could control the economy of countries, the waste it generates
must be handled with the utmost care and firmness to avoid any
possibility of sharing its secret structures with another partner
and production of fake money. However, the structure and compo-
sition of this waste should be known (or analyzed) for researchers
ELEB3 so that they were able to suggest the appropriate recycling tech-
ELEB2 nology, as we have been doing in the present research. Also, the
appropriate recycling technology of this type of waste cannot be
ELEB1 selected by researchers only; decision makers have to participate.
ELEB0 In this case, an optimal solution may be selected according to four
main factors (environmental, economic, yield or recycling rate, and
sustainability), at the same time keeping the composition of ban-
knotes structural safe. All these technical factors have been studied
300 350 400 situation has become clearer for decision makers and investors,
who can select the best solution between three different technolo-
gies developed by our team, including thermal treatment (pyroly-
sis), chemical treatment (leaching and dissolution), and biological
30
S. Yousef, N. Kuliešienė, S. Sakalauskaitė et al.
treatment. Also, when the present technology is compared to other
two technologies published by our team recently (Yousef et al.,
2019; Yousef et al., 2020), especially cotton recovery using chem-
ical technology, it was revealed that the safety factor is strongly
attended in the present technology, where biological technology
does not share any data related to structure, the amount of metals,
magnetic bar, and compositions of banknotes.
4. Conclusions
The authors of the present research have developed a new sus-
tainable biotechnology for recycling and conversion of end-of-life
euro banknotes (ELEBs) to glucose via submerged fermentation
and hydrolysis processes. The suggested strategy is composed of
five successive and parallel stages, including preparation of spore
media, cultivation, pretreatment of ELEBs, fermentation, and
upscale fermentation and hydrolysis processes. The results showed
that the milling coupled with leaching pretreatment had a signifi-
cant effect on the cellulase activity and glucose yield reached 12.97
FPU/g and 96%, respectively. These results demonstrate that the
proposed strategy has a great potential in bio-recycling of ELEBs
and that it may achieve the circularity and sustainability of the
euro banknote industry.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgements
This research was supported by the Research, Development and
Innovation Fund of Kaunas University of Technology (Project Grant
No. PP-88D/19). Acknowledgement must also be given to Dr. Erika
Adomavičiu tė, which supplied the research with end-of-life of Euro
banknotes.
Appendix A. Supplementary material
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.wasman.2021.01.007.
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