Journal of Cleaner Production 314 (2021) 128058

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Journal of Cleaner Production

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A new strategy for functionalization of char derived from pyrolysis of

textile waste and its application as hybrid fillers (CNTs/char and graphene/
char) in cement industry
Samy Yousef a, c, *, Regina Kalpokaitė-Dičkuvienė b, Arūnas Baltušnikas b, Inna Pitak b,
Stasė Irena Lukošiūtė b
a
Department of Production Engineering, Faculty of Mechanical Engineering and Design, Kaunas University of Technology, LT-51424, Kaunas, Lithuania
b
Laboratory of Materials Research and Testing, Lithuanian Energy Institute (LEI), Breslaujos 3, LT-44403, 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

Handling Editor: Prof. Jiri Jaromir Klemeš Char derived from pyrolysis of textile waste (CTW) represents about 18 wt% of pyrolysis products with smaller
economic value. In order to maximize the economic performance of CTW, this research aims to develop a sus­
Keywords: tainable strategy for reprocessing CTW into fine spherical carbon black (CB) particles that can be used as single
Textile waste or hybrid fillers (Carbon nanotubes (CNTs)/CB and graphene (GO)/CB) in cement composite applications. The
Pyrolysis
implementation of the suggested strategy was started by producing of CTW using a pyrolysis reactor, followed by
Char
refining of CTW using milling and chemical treatments to synthesize CB of 10–20 μm. The synthesized CB (0.05
Carbon black particles
Hybrid wt%) was used as a single filler and hybrid fillers (CNTs/CB and graphene/CB: 50/50) to enhance the properties
Cement paste of cement paste. Also, two other samples CNTs/cement and GO/cement were prepared for comparison. In case of
all the prepared cement matrixes, colloidal silica was used as a pre-dispersion medium to disperse the selected
fillers uniformly in the aqueous solutions. Besides, silica fume (25 wt %) was added during the mixing process to
facilitate dispersion and to increase the interfacial strength between fillers in cement paste. The morphology,
chemical structure, and composition of the treated char were observed using Scanning electron microscope
(SEM), Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, and inductively coupled plasma
mass spectrometry (ICP). Meanwhile, the compressive and flexural strengths of the prepared cement pastes were
tested according to standard EN 196-1 for 28 and 56 days. Also, the basic chemical and physical properties (X-ray
diffraction analysis (XRD), pore size distribution, etc.) and thermal behaviour (using Thermogravimetric) of
cement pastes were studied. The results showed that the treated char can be a strong competitor for both CNTs
and graphene, especially at longer curing time (56 day) with compressive and flexural strengths estimated at 82
and 12 MPa, respectively. Also, the hybrid paste (CNTs-CB) proved results almost similar to CNTs and GO, which
means that the treated char can be a sustainable alternative and a cheap filler, when compared to CNTs and GO.

1. Introduction represented by emissions and pollution, while the economic conse­

quences are represented by the amount of land consumed in the landfill
According to the international reports, more than 110 million tons of (Cesar da Silva et al., 2021). Therefore, decision makers rushed to take a
all apparel and textile fibres are produced annually around the world, set of measures to ensure that these consequences are overcome, making
what leads to generation of a huge amount of textile wastes (Li et al., the most of these wastes, reducing emissions by burying them, and
2020). Until recently, most of this waste was disposed of by burning, preserving the natural resources at the same time (Luo et al., 2021). The
incineration or landfill as a municipal solid waste (MSW) (Istrate et al., fundamental objective would be to focus on recycling practices of textile
2021), which were causing severe environmental and economic conse­ waste and its conversion into high value-added products (Xu et al.,
quences (Yasin and Sun, 2019). Theses environmental consequences are 2019). Since cotton and polyester are considered to be the basic

* Corresponding author. Department of Production Engineering, Faculty of Mechanical Engineering and Design, Kaunas University of Technology, LT-51424,
Kaunas. Lithuania.
E-mail address: ahmed.saed@ktu.lt (S. Yousef).

https://doi.org/10.1016/j.jclepro.2021.128058
Received 25 January 2021; Received in revised form 19 June 2021; Accepted 20 June 2021
Available online 23 June 2021
0959-6526/© 2021 Elsevier Ltd. All rights reserved.
S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

components of this waste (Subramanian et al., 2020a), it was a strong waste (CTW) is distinguished by a unique structure compared with chars
motivation for decision makers to insist on achieving maximum benefit derived from pyrolysis of other feedstock. For example, char derived
from these elements and recovering them in many forms. Also, many from pyrolysis of metallised food packaging plastics has a big amount of
strategies have been developed to separate textiles from MSW (Nørup aluminium (35 wt%) (Yousef et al., 2021b), hence needing additional
et al., 2019a). In addition, many systems have been developed for chemical leaching treatment to separate aluminium from carbon frac­
collection of old textiles in exchange for some financial incentives to tion (Yousef et al., 2019b). Meanwhile. the CTW consists mainly of the
urge the users to participate in the collection and sorting processes to carbon component loaded with a small number of dyes, which con­
facilitate recycling process (Nørup et al., 2018; Mäkelä et al., 2020). tributes to its faster and easier refining. In order to refine pyrolysis char,
Having collected and sorted used textiles, the good clothes are selected, Yousef et al. (2021c) used the milling treatment and the leaching process
washed, and sold as second-hand products (Nørup et al., 2019b), while to convert char into carbon black (CB) particles free from heavy metals.
the damaged clothes are shredded, then treated chemically to remove This approach may be promising in refining of CTW. As well, especially
dyes and impurities, and spunagain to produce yarns that can be used in since the leaching process is not necessary in this case because the major
production of fabric again (Haslinger et al., 2019). Despite the prom­ part of dyes is consumed during pyrolysis of textile waste as
ising results, this strategy has several limitations, such as non-uniform self-catalysts to accelerate the reaction and to increase the conversion
chemical composition, which affects negatively quality of the pro­ rate (Yousef et al., 2019a). Also, the functionalization process can be
duced fabrics (Ütebay et al., 2019). used to remove the impurities and amorphous phase and to modify
In order to maintain the chemical composition and to recover cotton surfaces of CB (Yousef et al., 2021b), thus synthesizing CB from a sus­
and polyester components individually, chemical treatments using tainable and cheaper source than commercial products. Additionally,
dissolution and leaching processes were developed (Yousef et al., 2019a, this functionalized CB can be used for many applications, including
2020a); however, these processes need a lot of chemicals and cement paste (Dong et al., 2020a), thus, closing the pyrolysis char loop
pre-treatments, which requires additional costs. Similar limitations also and realizing the concept of circular economy in the textile waste sector
appear in valorisation of textile waste using bio-recycling process and and the cement industry, too.
facilitating the recovery of glucose and polyester (Wang et al., 2018). In In order to adopt this strategy and to increase economic performance
addition, there are other restrictions related to high reaction time, low of CTW, CTW was upgraded and functionalized into CB in this work.
yield, selection of the suitable fungi, etc. (Subramanian et al., 2020b; Subsequently, the functionalized CB with a filling effect was used as a
Yousef et al., 2021a). To avoid these problems, pyrolysis was used to micro filler material to improve performance of cement paste compos­
convert these textiles into high-value energy products, including oil ites (Khan et al., 2017). In order to evaluate the developed strategy,
(38%), gas (44%), and char (18%) (Yousef et al., 2019b). Despite these another two sets of Carbon nanotube (CNTs)/cement paste, and gra­
promising results, pyrolysis treatment has some limitations similar to phene oxide (GO)/cement paste were prepared for comparison; espe­
burning and incineration, particularly high power consumption and gas cially, CB, CNTs, and GO were classified as having high carbon content
emission, etc. However, these shortages can be overcame through using and were used in many studies to improve the performance of cement
the obtained pyrolysis gas in operation of the pyrolysis plant and using paste (Şimşek, 2020; Qureshi and Panesar, 2020). Where these types of
reactors closed tightly to avoid any leakages during the decomposition filler materials are characterized by their higher surface-to-volume,
process. It is worth mentioning that the obtained oil and gas have many which leads to rapid interaction between cement paste bonds and
applications after having been upgraded as fuel, chemical sources, fillers followed by closing up of their pores, what contributes in
renewable energy sources, etc. (Yousef et al., 2020b, 2020c, 2021a), improving in their mechanical performance. Finally, another two sets of
while the obtained char has less economic benefit compared to oil and CNTs-CB/cement paste and GO-CB/cement paste were fabricated to
gas. However, char is classified by a high carbon content, large surface study the effect of CB hybrid on the cement paste’s properties and to
area, big porosity, chemical resistance, and it can be prepared at rela­ attempt to reduce the price of fillers, as well.
tively moderate temperature (Huang et al., 2020). Due to their compo­
sition and characteristics, char products have been used for several 2. Experimental
applications, including as solid fuel for energy sector, filler material for
asphalt, catalytic materials, production of dyes, pollutant removal, 2.1. Materials and chemicals
agriculture, cement, etc. (Zhou et al., 2020; Ahmed and Hameed, 2020;
Gupta and Kua, 2019). Textile waste (waste jeans) was collected from municipal solid waste
It is clear that char has been included in many industries as a sec­ in Kaunas, Lithuania. The collected textile waste was cut into small
ondary raw material of lesser value, due to the fact that the chemical, pieces of 10 mm × 10 mm to prepare the pyrolysis feedstock (200 g). All
physical, and morphological properties of char are not constant and gases and chemicals needed for pyrolysis treatment were provided by
change depending on the composition of feedstock and pyrolysis con­ the Lithuanian Energy Institute. The reagents used in char leaching and
ditions (e.g., nitrogen flow rate, heating rate, temperature, residence refining were bought from Sigma-12 Aldrich Corp. Portland cement of
time, etc.) (Tang et al., 2020). All of these variables result in a char with type CEM II/A-LL 42.5 N (PC) was supplied by JC Akmenes Cementas
irregular and random structure. Also, most of studies were focused on Lithuania; colloidal nanosilica GAIA (nSi) with 22 wt% of dry solid
finding optimum pyrolysis conditions that could increase the yield of oil content and pH 5 was supplied by Ulmen (Spain); silica fumes (SF) RW-
and gas (valuable products) without giving a lot of attention to the Füller with 96% of SiO2 were supplied by RW silicium GmbH. Finally,
char’s properties, what makes it difficult to find a clear relationship carbon nanotubes (CNTs) with 20 nm in diameter were synthesized
between the char’s properties and the reaction conditions (Balcik-Can­ using the CVD multi-quartz tubes and the high-resolution transmission
bolat et al., 2017). The same features were observed in chars derived electron microscopy (TEM) images are shown in Fig. (1A) (Yousef and
from torrefaction of textile waste using a mild pyrolysis treatment Mohamed, 2016). The GO sheets with 10 nm in thickness were syn­
(Hanoğlu et al., 2019). Therefore, the char derived from waste pyrolysis thesized using multi-roll milling devices by dispersing expandable
in general should be refined before using it for any high graphite in organic solvent with ratio 1:3 (W/W) at 500 rpm for 30 min.
tech-application. The refining or upgrading process of the char is defined After that the prepared suspension was fed into multi-roller wet milling
as a process reprocessing char into a raw material in the form of carbon unit for exfoliation process at 600 rpm for 45 min to produce the
black particles with uniform shape, size, and composition, hence facil­ as-prepared GO. Subsequently, the as-prepared GO was exposed to
itating its marketing and achieving high profits (Junqing et al., 2020; ultrasonication and centrifugation process to remove the exfoliated
Riva et al., 2020). particles (Yousef et al., 2018). The photos of the prepared GO taken by
Among all the char products, char derived from pyrolysis of textile the scanning electron microscope (SEM) are shown in Fig. (1B).

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

Fig. (1). A,B) TEM and SEM images of CNTs and GO, and C) XRD pattern of the synthesized CNTs and GO (Yousef and Mohamed, 2016; Yousef et al., 2018).

Figure (1C) shows the XRD pattern of the prepared CNTs and GO. It is particles (Qureshi and Panesar, 2020).
clear that both patterns manifest a strong reflection peak at 25.7◦ (CNTs)
and 25.8◦ (GO), which confirms that the synthesized particles are CNTs 2.2.2. Preparation and dispersion of fillers in aqueous solutions
and GO.
2.2.2.1. Selection of dispersion technique and concentration of filler
materials. As it is known, cement paste consists of a solid powder phase
2.2. Design of the research experiments
(cement powder) and an aqueous solution. Generally, there are two
ways to disperse filler materials in the cement matrix: dispersion of filler
The flowchart of the current experiments was designed in four main
materials in a solid phase or in an aqueous solution. The dispersion in a
stages: (I) preparation of pyrolysis char and its refining, (II) preparation
solid phase is usually performed using a ball mill, thus leading to
and dispersion of fillers (CB, CNTs, and GO)/aqueous solutions, (III)
breakage of the fillers under the impact of the collision of balls, which
fabrication of compressive and flexural samples of fillers/cement pastes,
has negative impact on the ratio of the fillers (e.g., CNTs, GO, etc.) (Shi
while the last stage was dedicated to characterize the mechanical,
et al., 2019; Visco et al., 2016). The dispersion in an aqueous solution is
chemical, and thermal of the fabricated cement matrix. All the disper­
easier and can be performed with the help of stirring or/and ultrasound
sion, fabrication, and characterization conditions are explained in detail
process (Ubertini et al., 2016). Also, a super-plasticizing process with the
in the following sections.
help of colloidal silica (nSi) is usually used to improve the dispersion
process and to avoid agglomeration of filler materials in the prepared
2.2.1. Production and refining of pyrolysis char
matrix (Chithra et al., 2016). Therefore, the dispersion in an aqueous
Waste jeans (200 g) were used as a feedstock for pyrolysis process.
solution was used in the present research. The super-plasticizer (1.25 wt
The conversion energy process was performed in a mini pyrolysis plant
% of cement) was mixed with cement powder fraction. What concerns
at a heating rate of 25 ◦ C/min up to 800 ◦ C for 44 min in nitrogen
concentration of filler materials, according to the literature, filler ma­
ambient (Yousef et al., 2019a). By the end of pyrolysis treatment, oil
terials, including CNTs, GO, CB, etc. with lower concentrations (≤0.05
(37.5 wt%), gas (44.7 wt%), and char (17.8 wt%) were received. In
wt%) can improve the mechanical performance of cement paste com­
order to upgrade the CTW (Fig. (2A)), the CTW fraction was exposed to
posite without causing agglomeration of particles (Vilela Rocha et al.,
two different consecutive treatments: milling treatment and chemical
2019; Li et al., 2018; Dong et al., 2019). Based on that, 0.05 wt% of
functionalization process. The milling process using Ball mill (mill
CNTs, GO, and CB were used in the present research as a filler material to
model Fritsch P-5) was used to convert CTW in the form of fibre needles
prepare the cement paste samples. Also, the hybrid CNTs-CB and GO-CB
into fine particles of uniform sizes. The milling treatment was performed
samples were prepared with the same concentration (0.05 wt%) and
at 20 Hz for 30 min until obtaining a high degree of fineness (Fig. (2B)).
with equal percentages (50:50).
Subsequently, the milled CTW was subjected to chemical functionali­
zation treatment to eliminate the exfoliated particles and impurities
2.2.2.2. Preparation of fillers/water-silica solutions. Fig. (3) shows the
(Fig. (2C)).
flowchart for dispersion of the selected fillers in aqueous solutions. As
The chemical treatment was performed at 125 ◦ C in the acidic
shown in the figure, in order to disperse the selected fillers (GO and CB)
mixture (Sulphuric acid: Nitric acid = 3:1) for 45 min (Yousef et al.,
and their hybrid fillers of the specified concentrations in aqueous solu­
2021b). Afterwards the filtration process by filter paper (pore size of 10
tions uniformly, at first the selected fillers were mixed continuously with
μm) was used to separate solid fraction from liquid phase in the prepared
nSi (0.6 g per 100 g of cement) using the magnetic stirrer at 1000 rpm for
milled CTW solution, thus obtaining the functionalized carbon black
30 min (Fig. (3A)) (Chithra et al., 2016). Afterwards, the prepared
particles after having left the solution overnight at 40 ◦ C for drying, as
suspensions were treated again using the ultrasonication process for 1 h
shown in (Fig. (2D)). In general, chemical treatment plays an important
to improve the dispersion (Fig. (3B)), thus preparing hydrophilic solu­
role in surface modification of particles, hence contributing to adhesion
tions capable of numerous hydrogen bonds with uniform distribution of
to cement matrix and decrease of agglomeration of the functionalized

Fig. (2). (A) Image of CTW (Yousef et al., 2019a), (B) sketch of milling process, (C) chemical functionalization treatment, and (D) image of the obtained func­
tionalized CB particles.

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

Fig. (3). Flowchart of dispersion of fillers in aqueous solutions.

filler materials (Fig. (3C)), which can enhance C–S–H microstructure filler in the prepared cement matrix composites, as illustrated in
after having been mixed with cement paste (Fraga et al., 2020; Du and Table 1.
Pang, 2019). Finally, tap water was poured into fillers/colloidal nSi
solutions just before their incorporation into the cement mixture and the 3. Characterizations
fillers were stirred mechanically for 3 min (Fig. (3D)). It was noticed that
CNTs cannot be mixed with nSi, therefore, nSi was replaced by iso­ 3.1. The treated pyrolysis char (CB)
propanol and then used as a pre-dispersion medium to disperse CNTs
under the influence of soundwave for 1 h (Rocha and Ludvig, 2020). The morphology and chemical composition of the obtained and
When preparing CNTs-CB and GO-CB hybrid solutions, at first 0.025 wt treated char were examined using the Scanning Electron Microscope and
% of GO or CNTs were mixed with nSi following the above-mentioned Energy-Dispersive X-ray Spectroscopy (SEM-EDS: Model ZEISS EVO
procedures, then CB were added into the GO or CNTs suspension and MA10), whereas Inductively Coupled Plasma-Optical Emission Spec­
mixed together using ultrasonication for 1 h at a lower frequency to troscopy (ICP-OES) was used to determine the precise concentration of
avoid overheating of the hybrid solutions (Du et al., 2020b). heavy metals in the treated samples. The ICP analysis was performed on
1 g of the untreated and treated samples and digested by aqua regia
2.2.2.3. Preparation of cement pastes. In order to improve and stabilize under ultrasonication treatment (Yousef et al., 2019c). The
the dispersion of the selected fillers in the fabricated cement composite Fourier-transform infrared spectroscopy (FTIR) and Raman spectros­
samples, 25 wt% of silica fumes (SF: related to cement weight) were copy were employed to observe the chemical structure of the treated
mixed with cement pastes in all the fabricated samples (Song et al., char (CB).
2020). The fabrication of composite samples was started with prepara­
tion of a reference paste sample for comparison. A reference sample was 3.2. Cement paste composites
prepared by mixing SF with cement in a dry state and adding subse­
quently the required amount of water pre-mixed with nSi at a The compressive and flexural mechanical tests of the prepared
water-to-cement ratio (w/c) 0.35, then mixing all the components cement composite batches were performed using the Zwick Roell uni­
together in a planetary type mixer for 3 min until the smooth paste was versal testing machine under loading rate of 0.5 mm/min according to
achieved, as shown in (Fig. (4A-C)) (Du and Pang, 2019). When pre­ standard EN 196-1 (European Standard EN 196). The measurements
paring the composite samples, the above procedures were followed, yet were performed on five samples from each batch after having cured
nSi-water solution was replaced by the specified filler (GO or BC) them for 28 and 56 days to check reproducibility of the results; then the
nSi-water solution. In case of CNTs and its hybrid, the CNTs dispersed in average values were taken to increase the accuracy of the obtained re­
isopropanol were mixed with the required amount of cement and left to sults and the tests were set up, are shown in Fig. (5A, B). The micro­
dry overnight. Then dry powder was mixed with SF in dry state, adding structure of the fracture surfaces was observed using SEM at 20 kV after
water-silica solution later. Finally, the obtained cement mixture was cast
into cubic 2 × 2 cm (compressive samples) and prismatic 2 × 2 × 10 cm
Table 1
(flexural samples) steel moulds and placed in a climate chamber at Codes of the prepared cement paste samples.
temperature (20 ± 1)◦ C and relative humidity (95 ± 5)%. The samples
Cement concentration 75 wt%
were removed from the moulds after 24 h and left to cure in the chamber
for the defined period, as shown in (Fig. (4C)). It is worth mentioning Silica fume 25 wt%
concentration
that cement paste samples are usually prepared according to the liter­
Filler types and – CB GO CNTs GO-CB CNTs-
ature and standards, with dimensions of 4 × 4 cm. However, due to concentrations (wt.%, CB
economic aspects, especially in the case of nanocomposites, these ge­ relative to total 0.05 0.05 0.05 0.025- 0.025-
ometries can be reduced, but with the same aspect ratio, what ensures weight) 0.025 0.025
that the geometry of the prepared samples is not affected, and that their Sample code CSF CB/ GO/ CNTs/ GO- CNTs-
CSF CSF CSF CB/ CB/CSF
surface properties are not significantly affected (Kalpokaitė-Dičkuvienė
CSF
et al., 2021). Each sample was given a code name based on the type of

Fig. (4). Flowchart of fabrication of cement paste samples.

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

Fig. (5). Set-up of (A,B) compressive and flexural tests, respectively, and (C) capillary imbibition test.

having coated them with gold to avoid reflection generated from high 4. Results and discussions
voltage. The capillary imbibition test was performed on broken pris­
matic samples according to EN 1015-18 (European Standard EN 1015). 4.1. Analysis of the treated pyrolysis char
Briefly, before starting the test, the tested samples were dried at 60 ◦ C
until a constant mass was obtained. Afterwards, the growth in mass Fig. (6A, B) shows SEM images of char derived from textile waste
change in the tested samples was monitored for specific time intervals, pyrolysis and the treated char, respectively. As it is illustrated, the
followed by determination of the amount of absorbed water as a capil­ received char (Fig. (6A)) is composed of individual microfibers with
lary imbibition capacity (mg/mm2) (Fig. (4C)). With regard to ther­ sharp edges and rough surfaces and contaminated by debris (indicated
mogravimetric analysis (TGA), the samples were crushed into powder by white circles) resulting from decomposition of cellulose, hemicellu­
and soaked in isopropanol for 20 min with afterwards drying in the oven lose, polyester, and lignin components into various compounds under
at 40 ◦ C for 15 min. TGA experiments were performed in the LINSEIS the applied pyrolysis temperature, including d-glucose, levoglucosan,
STA PT1600 thermal analyser in nitrogen at room temperature up to glucopyranose, etc. (Yousef et al., 2020d). After having treated the py­
1000 ◦ C and at heating rate of 15 ◦ C/min. Whereas cement paste fluidity rolysis char and having exposed it to grinding and chemical function­
was measured according to ASTM C 143 and the viscosity was estimated alization treatment, all microfibers became smoother and acquired with
by coaxial viscometer (Indukuri et al., 2020). Finally, the amount of a uniform size (10–15 μm) and shape (spherical particles), as shown in
portlandite (CH), hydration degree (HD), and chemically bound water Fig. (6B). Also, it was noted that debris and impurities disappeared, and
(wb) were calculated from the obtained TGA curves, using Eqs. [1–4], the abrasive particles became free-stream particles, what proof that
respectively (Kalpokaitė-Dičkuvienė et al., 2021). functionalization treatment has a significant effect on the morphology of
the obtained char.
(m410 x m490 ) x 4.11
CH = (1) In order to determine the correct composition and chemical structure
m490
of the obtained powder, FTIR analysis and Raman spectroscopy were
wb used. FTIR analysis (Fig. (6C)) showed that the treated powder spectra
HD = (2) contained only one sharp peak at 2362 cm− 1 because of C– – O bonding
0.24 x mc
(typical position of CO2). Meanwhile, the Raman spectra (Fig. (6D))
where m410 and m490 are the samples’ mass at 410 ◦ C and 490 ◦ C, showed that due to the characteristics of disordered band and graphitic
respectively, while mc represents the contained cement mass in the tested band, and receptivity, the tested sample contained two sharp peaks in
sample and can be calculated using Eq. [3]. the range 1360–1580 cm− 1. The presence of these peaks in FTIR and
mi Raman analysis indicates that the obtained powder was carbon particles
mc (3) containing few amorphous carbons and most of contaminations and
[(1 + w/c) x (1 + LOIc )]
undesirable elements were removed using the milling and chemical
where mi , w/c, and LOIc are initial mass of a sample, water-to-cement treatment (Wu et al., 2020; Saravanan et al., 2014). Finally, the ICP
ratio (0.35), and loss on ignition of cement, respectively, while the results showed that CB sample almost does not have any heavy metals, if
chemically bound water (wb) can be determined using Eq. [4], where compared with the untreated sample, which contained few metals, in
Ldh, Ldx, Ldc, and Ldca represent mass loss in dehydration, dehydrox­ particular, Cu (8.33 mg/L), Cr (1.43 mg/L), Ni (0.039 mg/L), Fe (26.3
ylation of Portlandite, decarbonation, and unhydrous cement, mg/L), Pb (0.68 mg/L), and Al (22.67 mg/L). This means that some of
respectively. these metals were used during the reaction as self-catalysts (Yousef
et al., 2019a), while the rest were leached from the derived char using
wb = Ldh + Ldx + 0.41(Ldc − Ldca ) (4) the applied treatments.

Fig. (6). A,B) SEM images of the untreated and treated solid residue, C) FTIR analysis of FCBs, and D) Raman spectroscopy of FCBs.

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4.2. Pore size distribution and capillary water absorption of cement Table 2
composites Influence of fillers on cement paste properties.
Sample code CSF CNTs/ GO/CSF CB/CSF GO-CB/ CNTs-
The pore size distribution of the fabricated cement composite is one CSF CSF CB/CSF
of the physical properties, which has a significant effect on the me­ Cement paste 255 79 74 72 66 69
chanical performance of the cement paste. This section studies the effect fluidity
of varying fillers and their hybrids on the pore size and their distribution (mm)
in the prepared pastes. Fig. (7A) shows the pore size distribution graphs Apparent 964 14,8456 14,5843 14,4267 12,5794 13,9461
viscosity
of the obtained samples of 2–50 nm diameter, which can be used to (mPa.s)
analyse the pores in the mesoporous region. Generally, these pores can Initial setting 160 120 125 128 125 130
be classified as harmful pores >50 nm, less harmful pores (20–50 nm) time (min)
and harmless pores (<20 nm) (Ying et al., 2020). It seems that all Final setting 270 231 235 231 238 240
time (min)
samples have almost the same trend and harmless pores make the ma­
jority with a pore size estimated at 4 nm with the following tendency:
CSF > GO/CSF > GO-CB/CSF > CB/CSF > CNTs/CSF > CNTs-CB/CSF, presence of fillers in the cement matrix led to decrease the fluidity and
indicating that CNTs/CSF, CNTs-CB/CSF, and CB/CSF can result in increase its viscosity in short setting time due to the interaction between
fewer harmful pores compared with CSF, GO/CSF, and GO-CB/CSF. In fillers and hydrated cement particles, what lead to accelerate of cement
terms of less harmful pores (20–50 nm), the tendency was changing a hydration and shortening of setting time. Also, it was observed that
little: CSF > GO-CB/CSF > GO/CSF > CB/CSF > CNTs-CB/CSF > CNTs/CSF, GO/CSF, and CB/CSF samples have almost similar perfor­
CNTs/CSF. Also, all these changes in pore size and structure were mance. While in case of hybrid samples, an apparent change was
affected by slit shape pores and production of calcium-silicate-hydrate noticted in the workability properties due to the electrostatic in­
(C–S–H) with varying percentages. Also, SF is classified as an teractions between cement particles and hybrid fillers and formed ag­
ultra-fine pozzolan that has a fast pozzolanic reaction and a greater filler gregation of cement composites due to the chemical cross-linking
effect in the pores (Fraga et al., 2020; Wu et al., 2020). This means that between the fillers and abundant divalent calcium cations in cement
fillers play major role in controlling pore size of cement paste and SF is (Indukuri et al., 2020), what lead to decrease the workability (in terms
an ideal candidate for refining their pores. Fig. (7B) shows the curves of of fluidity) and increase the mixing energy.
cumulative pore volumes versus pore width of the prepared pastes on
the 56th day. As shown in the curves, CNTs-CB/CSF, CB/CSF,
CNTs/CSF, and GO/CSF samples have a smaller quantity of pores, when 4.4. Mechanisms for incorporation of fillers and silica fume into the
compared with CSF and GO/CSF samples. Also, these results agree with cement pastes
the results in the literature, thus confirming that presence of CNTs and
GO in cement paste reduces quantity of harmful pores and increases As listed before, the prepared composites contained three main
number of harmless pores (Vilela Rocha et al., 2019; Dong et al., 2019). components: filler (single or hybrid), SF, and cement. Fig. (8) simulates
Fig. (7C) shows representative water absorption measurements of the distribution and incorporation of different fillers and SF into the
cement composites. As shown in the fitting data, as time increases, the cement pastes to understand the mechanisms of incorporation of filler/
contribution of capillary sorption to moisture intake increases gradually, SF cement composite. According to the proposed model, virgin cement
especially in CB/CSF and GO/CSF and their hybrid paste. Meanwhile, paste contains a lot of pores (air voids, capillary pores, and gel pores) of
CNTs-CB/CSF, CNTs-CB/CSF, and CSF samples manifest higher water irregular shape and random distribution. When SF was added to cement
resistance because sorptivity evaluation depends on the quantity of paste (Fig. (8B)), the size of these pores started decreasing due to
small capillary pores (<50 nm), including harmful, less harmful, and pozzolanic reaction of Portland cement and SF. When the curing time
harmless pores (Fraga et al., 2020). These results agree with measure­ was increased up to 56 days, most of SF particles were hydrated with
ments of pore size distribution and cumulative pore volume. Besides, it pozzolanic, thus producing more C–S–H crystals, which led to blocking
was observed that the cumulative pore volume of the hybrid the matrix pores and their internal microstructure a little (Fraga et al.,
CNTs-CB/CSF paste was lower than that of the GO sample due to 2020). As stated above, 0.05 wt% of fillers is considered to be an opti­
reduced Ca(OH)2 compound as a result of the pozzolanic reaction mum value, when they disperse uniformly inside of the cement matrix,
(Andrade Neto et al., 2021). causing smaller conglomeration. This uniform dispersion of GO, CNTs,
and CB inside of CSF pastes is simulated in Fig. (8C-E). Also, SF particles’
sizes are finer than those of fillers. Besides, they have higher
4.3. Workability properties surface-to-volume ratio, hence contributing to acceleration and
improvement of incorporation of fillers with CSF paste (Dong et al.,
Table 2 shows the effect of fillers on cement paste workability 2020b). In this case, the chemical bonds were formed on the outer
properties (e.g., fluidity, viscosity and setting time). It is clear that the surfaces of SF and GO, CNTs, or CB. In addition, some of these fillers

Fig. (7). (A) Pore size distribution of cement pastes, (B) Cumulative pore volume of cement pastes, and (C) Water sorption as a function of the square root of time for
cement composites.

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Fig. (8). Schematic plot of distribution of SF and fillers in cement paste composites.

deposited on the internal surface of pores during the solidification with portlandite (Du et al., 2020a).
process and acted as surface modifiers leading to close-up of the pores. After 56 days, it was noted that curing time had not affected the
These surfaces modifying fillers were characterized by a high selectivity compressive strength of CSF. In case of cement composite pastes, GO/
and absorption of gases, including N2, CO2, etc. (Yousef et al., 2020c, CSF and CB/CSF proved better performance compared with CNTs
Yousef et al., 2020e). (improvement by 13% (86) and 6% (82), respectively), when compared
In case of hybrid samples: GO-CB/CSF and CNTs-CB/CSF (Fig. (8F, with the same batches tested after 28 days. This is because GO and CB
G)), the bonding mechanism is somewhat complex due to formulation of have a larger surface area, which needs longer curing to achieve com­
many bonds between cement, SF, and hybrid fillers themselves (GO-CB plete incorporation with cement molecules and improvement of C–S–H
or CNTs-CB). For simplicity, in case of the hybrid samples, the study was characteristics. In case of hybrid (GO-CB/CSF and CNTs-CB/CSF) pastes,
focused on the bonds between the fillers (GO-CB and CNTs-CB) since the the compressive strength values were improved by 10% (76 MPa) and
other bonding existing in other samples had been discussed before 16% (81 MPa), respectively. This can be explained by hydration of GO-
(Fig. (8A-E)). In these hybrid samples, three types of fillers of different CB and CNTs-CB fillers occur as well as the hydration of cement paste,
sizes and shapes were used. GO and CNTs had smaller size (in the range hence leading to rearrangement of C–S–H molecular structure. As it is
10–20 nm) with high aspect ratio (surface area to volume), thus shown, the curing time plays a vital role in production of C–S–H,
contributing to rapid interaction and bonding on the surface of CB. enhancement of hydration and finer pore structure of the matrix
Although the chemical bonds in this case were also formed on the outer incorporated with fillers, where these elements are considered as the
surfaces of GO and CNTs, but CNTs had bigger surface area (circular main components hydrating the cement paste and at the same time, they
circumference higher) compared with GO (flat area), thus leading to are regarded as primarily responsible for cement’s strength (Seda­
better bonding between CNTs and CB (Yousef et al., 2016; Yousef et al., ghatdoost et al., 2019). In addition, after 56 days, the cumulative pore
2018). volume of CB sample was lower than that of GO and CSF samples
because of reaction of silicon dioxide with calcium hydroxide Ca(OH)2
4.5. Compressive strength of the cement pastes and decreased Ca(OH)2 amount, thus refining the pore structure in the
cement composites. Based on these results, in case of long curing time,
Fig. (9) illustrates the compressive strength results of cement paste CB/CSF paste has bigger compressive strength compared with Portland
composites after 28 days and 56 days. As shown in the figure, due to cement CSF (improved by 52% and 12%, respectively). Also, the used CB
decrease in the pore sizes of CSF and formulation of more C–S–H crys­ in the form of single filler or hybrid can be a strong competitor for GO
tals, after 28 days, the compressive strength of pristine sample (CSF) was and CNTs fillers with estimated compressive strength at 86 MPa
estimated at 74 MPa with 45% improvement, when compared with (GO/CSF and CNTs/CSF) and 82 MPa for CB/CSF and CNTs-CB/CSF
Portland cement paste (Fraga et al., 2020; Ahmadi et al., 2020). How­ pastes with reduction of 5%.
ever, introduction of GO, CB, and CNTs into CSF pastes increased
compressive strength by 3% (76 MPa), 5% (78 MPa) and 14% (84 MPa),
respectively, compared with CSF. This slight improvement is due to the 4.6. Flexural strength of the cement pastes
fact that these fillers help to refine the pore structure of the cement
paste, which results in acceleration of the pozzolanic reaction and Fig. (10) shows the flexural strength results of the cement pastes
closing or Stenosis of the voids and its reduced porosity (which acts as reinforced by CNTs, GO, BC, and their hybrids (GO-CB and CNTs-CB)
cavitation and cracks affected negatively on the size of solid areas) (Song after 28 days and 56 days. Similarly to the compressive strength re­
et al., 2020; Li et al., 2020; Alobiedy et al., 2019). On the contrary, in sults after 28 days, the addition of SF to cement had a significant effect
case of hybrid (GO-CB and CNTs-CB) pastes, the recorded strength on flexural strength results, where the strength of Portland cement
showed a slight decrease estimated at 8% (68 MPa) and 5% (70 MPa) as increased from 5.3 MPa (Chaipanich et al., 2017) to 9.12 MPa (improved
a result of presence of several fillers with different particles sizes and by 90%) due to enhanced C–S–H and hydration behaviour. Meanwhile,
shapes that need longer curing time to hydrate these fillers and react

Fig. (10). Flexural strength of the fabricated cement pastes at 28 and 56-
Fig. (9). Compressive strength at different age time (28 and 56 days). day age.

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

the flexural strengths of GO/CSF, CB/CSF, and GO-CB/CSF pastes had pores, etc., thus enhancing the strength and durability of cement ma­
not been changed by additives due to smaller C–S–H reaction between terials and these results agree with the pore size distribution described in
cement and fillers. CNTs/CSF (13.2 MPa) and its hybrid CNTs-CB/CSF Section 4.2.
(12.7 MPa) pastes showed better performance with improvement by
42, 24, and 39%, respectively, due to the high aspect ratio and smaller 4.8. XRD analysis
surface area leading to fast incorporation of cement and CB and bigger
rigidity of the fabricated samples (Silvestro and Jean Paul Gleize, 2020; Fig. (12) shows the XRD patterns of the hardened cement pastes
Subadra et al., 2020). After 56 days, the flexural strengths of CB/CSF and (after grounding into powders in a mortar) after 56 days of curing. As
its hybrids GO-CB and CNTs-CB were increased significantly by 36%, shown in the XRD pattern, several peaks were observed in all the cement
21%, and 9%, respectively (when compared with the same batches after pastes with different intensity: portlandite (Ca(OH)2) at 18◦ , silicates
28 days) and these results agree with the compressive strength results in and calcium carbonate (CaCO3) at 29.6◦ , silicates and ferrite and
the above section. This significant improvement is manifested in CB/CSF ettringite at 32◦ , portlandite and silicates at 34.5◦ , silicates and calcium
sample in particular because of big rigidity of CB (Dong et al., 2020c). carbonate at 39.6◦ , CaCO3 at 41.3◦ , portlandite at 48.6◦ , 52◦ , 57◦ , and
Finally, it seems that CB as a filler and a hybrid has better flexural 62◦ . As it is shown, in addition to several CaCO3 compounds, portlandite
performance than GO with improvement of 23% (CB/CSF), 17% represents the main compound resulting from carbonation of Ca(OH)2
(GO-CB/CSF), and 31% (CNTs-CB/CSF), when compared with GO/CSF generated from hydration and anhydrous CaCO3 (Jeong et al., 2020).
after 56 days of curing. However, the intensity of these peaks shows some qualitative differences
due to the incorporation of different fillers, especially at 29.6◦ (silicates
4.7. Fracture surface morphology and calcium carbonate). The intensity of this peak increased a little in
CNT/CSF and CNTs-CB/CSF samples, thus leading to increased number
Fig. (11) shows SEM images of fracture surface morphology of the of crystallized compounds in the fabricated cement (Leonavičius et al.,
cement paste composites with scale 1 μm at 20 KV. The observation 2020; Pârvan et al., 2020). Also, the characterised peaks of CNTs, GO,
process was focused on the samples hydrated for 56 days. Fig. (11A) and CB disappeared when the filler was incorporated with the cement
shows the SEM image of cement paste incorporated with SF particles. It mix. In addition, the amount of the dispersed fillers in cement pastes was
is clear that SF particles are dispersed uniformly with smaller SF ag­ very small (0.05 wt%), thus making it difficult to be identified with the
gregations in cement paste. Also, the crystals of portlandite are help of XRD.
distributed well with some formed crystal faces. These features are
similar to the texture obtained by (Ni et al., 2021). Regarding the 4.9. TGA-DTG analysis
composite samples, it seems that CNTs (needle-like) and SF are dispersed
well in the prepared paste (CNTs/CSF) with strong incorporation with Fig. (13A-B) shows thermogravimetric (TGA-DTG) curves of the
cement paste (Fig. (11B)). Also, the portlandite crystals were switched prepared cement pastes after 56 days of curing. As shown in the TGA
from large masses to thin flaks formation of ettringite in the pore space curves (Fig. (13A)), all samples have almost the same features with re­
and their surfaces were refined. The features were observed in case of gard to the number of items in the decomposition zones, where the
CB/CSF paste (Fig. (11C)), but the needle-like particles were replaced by curves were composed of four degradation zones distributed in the form
a huge number of well-distributed spherical particles. In case of GO/CSF described below. The first zone started from room temperature up to
paste, as show in Fig. (11D), GO layers are represented by folded and 200 ◦ C with weight loss of 12% due to vaporization of free water and
wrinkled texture and destroyed lamellae resulting from the high shear other organic components in plasticizer (Jialuo He et al., 2017), and this
load generated during the fracturing process (Bai et al., 2018). However, zone was almost constant in all the tested samples. The second weight
these destroyed lamellas distributed homogeneously on the surface of loss zone appeared because of Ca (OH)2 decomposed in the course of
cement grains. In case of hybrid GO-CB/CSF and CNTs-CB/CSF pastes dihydroxylation of in the region of 200 ◦ C and 470 ◦ C with weight loss in
(Fig. (11E, F)), CB precipitated on the surface of CNTs or GO and bond the range of 3–5 wt%. Meanwhile, the third decomposition zone was
together using chemical bonding, as explained in before in Section 4.3. associated with the breakdown of Ca(OH)2 at a temperature between
These results confirm that SF and nSi succeeded to disperse the selected 470 ◦ C and 765 ◦ C with weight loss of 3–6 wt% (Lilkov et al., 2012).
fillers in cement pastes uniformly. Also, the observation process showed Finally, the last weight loss was associated with the filler materials
that the prepared pastes contained few air voids, capillary pores, and gel decomposed from 765 ◦ C until the end with weight loss estimated at 3%.

Fig. (11). SEM images of (A) cement, (B) CNTs, (C) GO, (D) CB, (E) CNTs/CB, and (F) GO/CB samples.

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

Fig. (12). XRD analysis of the cement pastes.

Fig. (13). A, B) TGA-DTG analysis of cement paste composites.

As it has been shown, up to 765 ◦ C, GO/CSF sample had higher thermal including making of chemicals, lubricants, fuel, etc. (Yousef et al.,
stability (20 wt%), while CB/CSF and CNTs-CB/CSF provides smaller 2021d, Yousef et al., 2021e). Meanwhile, the synthesized gas can be
thermal stability estimated at 22 wt% due to the high thermal stability of used as a fuel gas after each gas (H2 and CH4 against CO2 compound) is
GO compared with CNTs and GO (Bai et al., 2018). Since the fabricated separated individually using membrane technology or any other
cement pastes contained many components (e.g., cement, SF, filler, chemical technology (Eimontas et al., 2021).
plasticizer, etc.), DTG results (Fig. (13B)) showed that all the tested Finally, by the end of char’s treatment, the received raw material can
pastes had four decomposition peaks at 131 ◦ C, 450 ◦ C, 351 ◦ C, 750 ◦ C, be used as a cost-effective filler material for several applications, thus
and 840 ◦ C because all these components had decomposed in the form of leading to closed loop pyrolysis of textile waste and protection of our
several sequentially reactions and these results agree with the TGA re­ environment, what contributes to keeping the climate and growth eco­
sults. Also, moderate shifting and rise in the maximum decomposition nomic profitable. Also, this strategy can be classified as a sustainable
temperature appeared because of slower or faster crystallization rates conversion technology with conversion rate of >81% and char yield of
with changing filler type (Lilkov et al., 2012; José et al., 2021). 18% with total utilization rate of 99% (Yousef et al., 2019d). Also, the
synthesized energy and materials have high quality, almost like the
commercial products, thus they preserve the resources. This means that
4.10. Integration of the suggested strategy into circular economy concept the capacity of remanufacturing principle was achieved in the suggested
strategy. Therefore, according to the aforementioned results, the sug­
Despite of the huge amount of generated textile waste and many gested strategy can be classified as an eco-friendly sustainable strategy
recently developed solutions, the integration of textile waste into the with high economic potential and it can help to move forward to the
Circular Economy (CE) system is mainly constrained by several chal­ Circular Economy and to close the loop of textile waste and cement in­
lenges: a) high conversion rate of the developed technology or recycling dustry, hence achieving compatibility between these two sectors as
rate of the suggested strategy, b) status of the recovered materials or shown in Fig. (14).
products, and ability to remanufacture them using the traditional and
advanced processes (Xu et al., 2019; Luo et al., 2021). All these factors 5. Conclusions
have been taken into consideration in the proposed strategy in the
current research, where at the end of the pyrolysis of textile waste, three In the present research, the authors have suggested a new sustainable
types of raw material and energy products were received: char, gas, and strategy for functionalization of char derived from pyrolysis of textile
oil. The obtained oil product can be used for several applications,

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S. Yousef et al. Journal of Cleaner Production 314 (2021) 128058

Fig. (14). Integration of the suggested strategy into Circular Economy.

waste (CTW) and used as single and hybrid fillers in cement industry. CRediT authorship contribution statement
The CTW was produced using a pyrolysis reactor, then exposed to
milling and chemical-functionalization treatment for size reduction and Samy Yousef: Conceptualization, Data curation, Formal analysis,
conversion of the decomposed fibres into micro spherical particles (CB) Funding acquisition, Investigation, Methodology, Project administra­
with less of amorphous carbon impurities. The functionalized particles tion, Resources, Software, Supervision, Writing – original draft, Writing
were used to refine the pores of cement paste and to improve its – review & editing. Regina Kalpokaitė-Dičkuvienė: Conceptualiza­
compressive and flexural strengths in presence of colloidal silica and tion, Data curation, Formal analysis, Funding acquisition, Investigation,
silica fume. Also, CB particles were mixed with CNTs and graphene (GO) Methodology, Project administration, Resources, Software, Supervision,
and used as hybrid fillers (CNTs-CB and GO/CB) in cement paste fol­ Writing – original draft, Writing – review & editing. Arūnas Bal­
lowed by studies of the effect of hybrid on cement paste properties. The tušnikas: Formal analysis. Inna Pitak: Data curation, Formal analysis.
experimental results and analysis highlighted the following: Stasė Irena Lukošiūtė: Formal analysis.

(A) The mechanical and chemical treatment can be used in general to Declaration of competing interest
treat the pyrolysis char, including CTW and its reprocessing into
micro spherical particles. The authors declare that they have no known competing financial
(B) Colloidal silica and silica fume can be used to disperse CB in interests or personal relationships that could have appeared to influence
cement paste using a magnetic stirrer and ultrasonication with the work reported in this paper.
uniform distribution.
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