coatings
Article
Multiwalled-Carbon-Nanotubes (MWCNTs)–GPTMS/
Tannic-Acid-Nanocomposite-Coated Cotton Fabric for
Sustainable Antibacterial Properties and Electrical Conductivity
Marwa M. Abd El-Hady 1,2, *, Asmaa Farouk 1,3






Citation: Abd El-Hady, M.M.;
Farouk, A.; Sharaf, S.
Multiwalled-Carbon-Nanotubes
(MWCNTs)–GPTMS/Tannic-Acid-
Nanocomposite-Coated Cotton
Fabric for Sustainable Antibacterial
Properties and Electrical
Conductivity. Coatings 2022, 12, 178.
https://doi.org/10.3390/
coatings12020178
Academic Editors: Arũnas
Ramanavičius and Alessandro
Pezzella
Received: 9 December 2021
Accepted: 24 January 2022
Published: 30 January 2022
Publisher’s Note: MDPI stays neutral
with regard to jurisdictional claims in
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iations.
Copyright: © 2022 by the authors.
Licensee MDPI, Basel, Switzerland.
This article is an open access article
distributed under the terms and
conditions of the Creative Commons
Attribution (CC BY) license (https://
creativecommons.org/licenses/by/
4.0/).
Coatings 2022, 12, 178. https://doi.org/10.3390/coatings12020178
and Samar Sharaf 1
1 National Research Centre, Textile Research and Technology Institute, 33 El-Behoth Street, Dokki,
Cairo P.O. Box 12622, Egypt; asmaa.saleh2015@yahoo.com (A.F.); samarsami2004@yahoo.com (S.S.)
2 Department of Physics, College of Science and Arts in Al-Asyah, Qassim University,
Buraidah 51452, Saudi Arabia
3 Department of Chemistry, Faculty of Science, King Khalid University, Abha 62529, Saudi Arabia
* Correspondence: m.aish@qu.edu.sa
Abstract: We propose a method of crosslinking multiwalled carbon nanotubes (MWCNTs) with
cotton fabric. 3-Glycidoxypropyltrimethoxy silane (GPTMS) polymer was used for the stabilization
and modification of the surfaces of MWCNTs. The presence of tannic acid in the finishing formulation
adds a sustainable functionality to the treated surface. The formation of the GPTMS–MWCNTs
nanocomposite as well as the MWCNTs–GPTMS tannic-epoxy nanocomposite on the fabric surface
was confirmed by Fourier-transform infrared spectra (FTIR). The surface morphology and physical
properties were investigated. An assessment of antibacterial activity, UV-protective properties,
and electrical conductivity was performed. The post-treatment results of the MWCNTs–GPTMS
nanocomposite fabric with tannic acid exhibited superior antibacterial character with the highest
inhibition zones for Staphylococcus aureus and Escherichia coli (26 mm, 24 mm). On the contrary,
the electrical conductivity was negatively impacted. The treatment of cotton fabric with tannic
acid showed a great UV-protection-factor estimation of 96.2, which was additionally improved by
treatment with MWCNTs 152.1. Cotton fabric treated with cotton/GPTMS/tannic acid/MWCNTs as
well as cotton/GPTMS/MWCNTs recorded the highest electrical-conductivity properties. Fabrication
of MWCNTs–GPTMS/tannic-acid-nanocomposite-coated cotton fabric for durable antibacterial and
UV protection with improved electrical and physical properties was successfully achieved.
Keywords: cotton fabric; MWCNTs nanocomposite; tannic acid; antibacterial properties; electrical
conductivity; GPTMS polymer
1. Introduction
Nanomaterials are used to design smart textiles for improving the properties of tex-
tiles such as wound healing, self-cleaning and military application [1–4]. Additionally, the
utilization of nanomaterials is beneficial for the enhancement the physical characteristics of
textiles in fields such as antibacterial-feature, water-repellence, soil-resistance, antistatic,
anti-infrared, and fire-retardant characteristics [5–8]. The use of nanomaterials not only
allows for the sufficient durability of fabrics but also has no impact on the fabric’s breatha-
bility or hand feel. This is because of the great surface-area-to-volume ratio and high
surface energy of nanoparticles [9,10].
The binding of nanoparticles to cellulosic substrates occurs via a crosslinking process.
Non-formaldehyde crosslinking agents such as 1,2,3,4-butanetetracarboxylic acid (BTCA),
citric acid, succinic acid, and maleic acid are employed for this function. The fixation
mechanism is explained through the molecular incorporation of the phosphorus catalyst in
the structure of the crosslinking agent followed by the formation of an ester linkage with
the cellulosic chains of the cotton [11,12]
https://www.mdpi.com/journal/coatings
Coatings 2022, 12, 178 2 of 14

Tannic acid (TA) is a natural product with ten gallic-acid molecules connected to
a central glucose unit [13]. It is isolated from naturally occurring resources (plants of
both herbaceous and woody kinds). Tannic acid has many outstanding properties. It has
antimutagen and antitumor characteristics. It is active against micro-organisms (bacteria
and viruses). Tannic acid, in the same way as phenolic acid, is classified in a polyphenolic
group. Many surveys have been reported on the use of tannic acid as an additive to
biopolymers, collagen, and polysaccharides such as chitosan, agarose, and starch as a
result of its unique characteristics. On the one hand, it exhibits an antimicrobial and
antiviral effects; it also indicates outstanding biological properties, namely improving cell
proliferation, tissue regeneration, and wound-healing procedures [14].
Carbon nanotubes (CNTs) are one of the most durable materials known. The tensile
strength of multilayer nanotubes is 63 GPa, which is much higher than that of hardened
steel (1.2 GPa). CNTs have a low density of only 1.3–1.4 g/cm3 . The high tensile strength
paired with the low density makes the use of CNTs highly desirable in various fields.
The characteristic properties of carbon nanotubes (CNTs), particularly their heat
conduction, electrical conductivity, high modulus of elasticity, high strength, and resistance
to chemicals, have resulted in the widespread application of CNTs.
The incorporation of CNTs into polymers has exhibited extraordinary electronic,
thermal, and mechanical properties as well as chemical and physical properties [15].
More recently, simple dip-coating, drying or exhaustion methods have been used for
the deposition of carbon nanotubes onto fabrics while different polymers have been used
as stabilizers [16,17]. Earlier studies have argued that polymeric composites that have
incorporated CNTs possess satisfactory physical, chemical, and mechanical properties [18].
Due to the fact that there is no interaction between the surface of textile fabrics
and carbon nanotubes, previous studies have reported the necessity of using network-
based polymers for dispersing and fixing CNTs on their surfaces. B. S. Shim et al. used
poly-4-styrene sulfonate (PSS) to disperse CNTs followed by the dipping of cotton fabric,
resulting in a conductive fabric that can be applied to telemedicine sensors and the detection
of albumin [19]. M. in het Panhuis et al. used aqueous sulfonated polyaniline to disperse
CNTs and used it as a dye for the prepared conductive textiles [20,21]. In another study,
P. Xue, K. et al. used a wet-spinning technique for the coating of cotton fabric with a
poly-vinyl alcohol/carbon-nanotube nanocomposite with the aim of developing yarns
with conductive applications [20]. Water-soluble carbon nanotubes were functionalized in
alkali and acidic solutions and then incorporated into a poly-vinyl alcohol (PVA) network
followed by the coating of a polypropylene thread in order to improve its mechanical
properties [21]. Recently, CNTs were dispersed in poly-vinyl pyrrolidone (PVP) medium
and deposited onto cotton fabric using a curing method under UV-C irradiation [22]. In
another recent study, a conductive super-hydrophobic cotton fabric was developed by
assembling carboxylated and aminated multiwalled carbon nanotubes and modifying them
with polydimethylsiloxane [23].
MWCNTs have been coated onto cotton fabrics by different methods for various
functionalities, i.e., super-hydrophobicity, self-cleaning and flame retardancy, as well as
improved mechanical resistance, electrical conductivity, and UV protection [24,25]. Dura-
bility plays a key role in the monitoring of the acquired properties. It was also reported that
many carboxylic acids have been used to crosslink CNTs with cotton fabric, i.e., succinic
acid as well as 1,2,3,4-butanetetracarboxylic acid (BTCA) [17,26].
To the best of our knowledge, there is no study on the crosslinking of MWCNTs with
cotton fabric using GPTMS polymer and tannic acid. Herein, a MWCNTs–GPTMS/tannic-
acid nanocomposite was fixed onto the surface of cotton fabric via crosslinking. GPTMS
polymer was used as a stabilizing and to modify the surfaces of the MWCNTs. Additionally,
it acted as a crosslinking and bridging agent for the enhancement of the deposition and
fixation of the nanocomposite onto the fabric. The use of tannic acid is not only environ-
mentally friendly and cost effective but also provides biocompatibility between MWCNTs
and GPTMS and enhances the antibacterial activity of the treated fabric without affecting
Coatings 2022, 12, 178 3 of 14

the physical and mechanical properties of the coated cotton fabric. Electrical properties
and antibacterial activity were also investigated.

2. Experimental
2.1. Materials
Mill-bleached pure 100% cotton fabric (138 g/m2 ) was supplied by Misr Company for
Spinning and Weaving Mehalla, El-Kobra, Egypt.

2.2. Chemicals
3-Glycidoxypropyltrimethoxy silane (GPTMS) with a purity of 98% (supplied by
Aldrich), The multiwalled carbon nanotubes (MWCNTs) were purchased from Nanotech
Port Co. Ltd. (Shenzhen, China) Their purity was >95%, their length was about 10 m and
their average outer diameter was 10–30 n.

2.3. Preparation of GPTMS Sol

A volume of 10 mL of GPTMS were dissolved in 100 mL ethanol before hydrolyzation
using 0.01 M hydrochloric acid. The resulting solution was stirred for at least 3 h to form
the base solution.

2.4. Coating of Fabrics Using MWCNTs–GPTMS Nano Sol

GPTMS solution was mixed with an MWCNTs suspension in an ethanolic solution.
1-methylimidazol (0.5 mL/10 mL GPTMS) was added as a catalyst. Fabric samples were
first immersed in ethanol and sonicated for 15 min to remove organic material and detergent,
then washed with distilled water and dried at 100 ◦ C; the fabric was then dipped in
MWCNTs-based solutions, each dip for 2 min. The treated samples were then dried at
80 ◦ C and cured at 130 ◦ C for 3 min. Finally, all samples were washed with deionized water
several times and dried.

2.5. Coating of Fabrics Using GPTMS/MWCNTs/Tannic Acid Nanocomposite

Clean cotton fabric was immersed in ethanol and sonicated for 15 min to remove
organic material and detergent, then washed with distilled water and dried at 100 ◦ C;
the fabrics were first dipped in solutions of tannic acid then in GPTMS–MWCNTs–based
solutions, each dip for 2 min. The treated samples were then dried at 80 ◦ C and cured at
130 ◦ C for 3 min. The second treatment was a post-treatment of the GPTMS–MWCNTs
fabric samples with tannic acid that involved being dried at 80 ◦ C and cured at 130 ◦ C for
3 min. Finally, all samples were washed with deionized water several times and dried.

3. Characterization
3.1. Fourier-Transform Infrared Spectroscopy (FTIR)
FTIR spectroscopy has been widely used in cellulose research. Because it is a very
simple means of acquiring direct information on chemical changes that occur during
various chemical treatments. ATR-FTIR equipment (Model IR 4700, JASCO, Tokyo, Japan)
was used to scan from 4000 to 400 cm−1 in ATR mode with KBr as a support material.
The software was set up to scan the background and samples at a specific number of
scans (64) and at a specific resolution (4).

3.2. Scanning Electron Micrograph SEM/EDX Analysis

Samples for SEM/EDX were taken using FEI INSPECTS Company, Philips, Holland
environmental scanning without coating. The elemental constitution of solid samples was
investigated using elemental micro-probe and elemental distribution-mapping techniques.
To provide a rapid quantitative and qualitative examination of the elemental composition,
a SEM equipped with an energy-dispersive spectroscope (EDX) with accelerating voltage
of 30 kV FELCO Netherland was used to perform elemental analysis of the particles.
Coatings 2022, 12, 178 4 of 14

3.3. Antibacterial Test

The antibacterial activity of the treated samples against Staphylococcus aureus, Bacil-
lus subtilis (G + ve), Escherichia coli, and Pseudomonas aeruginosa (G − ve) bacteria
was determined using an agar plate. The antibacterial activity of the fabric samples was
evaluated using (ATCC 1533) the disk-diffusion method [27,28].

3.4. UV Protection Factor

Ultraviolet-protection factor (UPF) was measured using an ultraviolet JASCO model
V-750 UV/VIS Spectrophotometer apparatus (JASCO, Tokyo, Japan). UV protection and
classification according to AS/NZS 4399:1996 were evaluated. The scanning range was
200–600 nm.

3.5. Electrical Conductivity Properties

A digital multimeter was used to measure the electrical conductivity of the dry textile
composite at room temperature (25 ◦ C). An electrical circuit consisting of a Hewlett Packard
6634B system DC power supply and a digital Hewlett Packard 34401A multimeter (Hewlett-
Packard Company, Palo Alto, CA, USA) was used to record electrical measurements.
Test Method 76-1995 of the American Association of Textile Chemists and Colorists
was used to conduct the measurements [29,30].

L
R = RS = ρ
A
RA
=ρ
L
1 L L
σ= = =
ρ RA RWt
where R = resistivity, Rs = bulk resistivity of fabric, L = length of fabric, σ = conductivity,
ρ = resistivity, A = cross-sectional area of the fabric, and W and t are width and thickness
of the fabric.

3.6. Tensile Strength

The tensile strength of the fabric samples was determined by the ASTM Test Method
D-1682-94 (1994). Two specimens for each treated fabric were tested in the warp direction
and the average value was recorded to represent the fabric-breaking load (Lb).

3.7. Roughness
Surface roughness was monitored according to the JIS 94 standard, using a surface-
roughness-measuring instrument SE 1700a made in Japan.

3.8. Statistical Analysis

Results were expressed as a mean value with its standard deviation (mean ± SD) of
each sample that was repeated three times (n = 3).

4. Results and Discussion

4.1. Mechanism of Deposition for MWCNTs–GPTMS-Tannic Nanocomposite on Cotton Fabric
Figure 1 depicts the mechanism diagram whereby tannic acid/MWCNT nanocom-
posites were deposited and attached to the cotton fabric. Due to the hydrophobic nature
of MWCNTs and their aggregation in an aqueous solution, GPTMS was added to the
modified MWCNT surfaces in order to enhance their hydrophilicity [31]. GPTMS was
pre-hydrolyzed for the conversion of the alkyl oxygen groups (–OCH3) to hydroxyl groups
(-OH) (equation (1) in Figure 1a). After its addition, stable hydrogen bonds were formed
between hydroxyl groups covering the surface of the MWCNTs and hydroxyl groups of
the hydrolyzed GPTMTs (equation (2) in Figure 1a). In the next step, cotton fabric was
 Figure 1 depicts the mechanism diagram whereby tannic acid/MWCNT nanocompo-
sites were deposited and attached to the cotton fabric. Due to the hydrophobic nature of
MWCNTs and their aggregation in an aqueous solution, GPTMS was added to the modi-
fied MWCNT surfaces in order to enhance their hydrophilicity [31]. GPTMS was pre-hy-
Coatings 2022, 12, 178 drolyzed for the conversion of the alkyl oxygen groups (–OCH3) to hydroxyl groups (- 5 of 14
OH) (equation (1)). After its addition, stable hydrogen bonds were formed between hy-
droxyl groups covering the surface of the MWCNTs and hydroxyl groups of the hydro-
lyzed GPTMTs (equation (2)). In the next step, cotton fabric was immersed in the previous
immersed in the previous nanotube solution followed by drying. MWCNTs–GPTMS was
nanotube solution followed by drying. MWCNTs–GPTMS was fixed onto the fabric by
fixed onto the fabric by ether crosslinking with the cotton fabric via the reaction of the
ether crosslinking with the cotton fabric via the reaction of the epoxy groups of GPTMS
epoxy groups of GPTMS with the hydroxyl groups of the cellulose structure, resulting in a
with the hydroxyl groups of the cellulose structure, resulting in a soft coat on the surface
soft(equation
of the fabric coat on the(3))surface of thethe
[32]. During fabric
last (equation (3) in Figure
stage, the treated fabric 1a)
was[32]. Duringinthe last stage,
immersed
a tannic-acid solution using a pad–dry–cure technique. At this stage, tannic acid was ad- technique.
the treated fabric was immersed in a tannic-acid solution using a pad–dry–cure
At this
sorbed onto the stage, tannic
surface acid
of the was adsorbed
modified MWCNTs, ontoresulting
the surface of the
in the modifiedofMWCNTs,
formation the result-
ing in the formation of
MWCNTs–GPTMS/tannic-acid the MWCNTs–GPTMS/tannic-acid
nanocomposite (equation (4)). This can nanocomposite
be explained in (equation (4)
in Figure
terms of the 1a). This
combination can be
between theexplained in termsring
aromatic benzene of the combination
in the tannic-acid between
molecule the aromatic
benzene ring
with the π-electron orbitinperpendicular
the tannic-acid molecule
to the MWCNT’s withaxial
thedirection,
π-electron orbit perpendicular
leading to a π–π to the
MWCNT’s axial direction, leading to a π–π electron interaction
electron interaction [33,34]. In the case of pretreatment with tannic acid, it could be ad- [33,34]. In the case of pre-
treatment with tannic acid, it could be adsorbed onto the surface
sorbed onto the surface of cotton fabric due to its hydrophilic hydroxyl groups, which of cotton fabric due to its
hydrophilic hydroxyl groups, which make hydrogen bonds
make hydrogen bonds with hydroxyl groups of cotton fabric. Additionally, GPTMS al- with hydroxyl groups of cotton
lows the fabric. Additionally,
homogeneous GPTMS
distribution of allows
MWCNTs the homogeneous
within its formed distribution
network, of MWCNTs
while the within its
hydroxylformed
groups network, while
of the tannic themay
acid hydroxyl
react groups
with GPTMSof the by
tannic acid may react
a ring-opening with GPTMS by a
addition
reaction, ring-opening
resulting in theaddition
fixation reaction, resulting in the
of the nanocomposite fixation of the nanocomposite [15,35].
[15,35].

ER REVIEW 6 of 14

(a)

(b)
Figure 1. (a) Schematic mechanismFigure
for deposition of MWCNTS–GPTMS/tannic
1. (a) Schematic acid of
mechanism for deposition nanocomposite
MWCNTS–GPTMS/tannic acid nanocomposite
on the surface of cotton fabric; (b)on
Structure of tannic acid.
the surface of cotton fabric; (b) Structure of tannic acid.

4.2. IR Analysis
The presence of functional groups on the modified cotton surface was confirmed
through Fourier-transform infrared spectra. Figure 2 shows FTIR spectra of the unmodi-
fied cotton (a), cotton fabric modified with the GPTMS–MWCNTs nanocomposite (b) and
cotton fabric modified with MWCNTs–GPTMS-tannic nanocomposite (c). On account of
 (b)

Coatings 2022, 12, 178 Figure 1. (a) Schematic mechanism for deposition of MWCNTS–GPTMS/tannic acid nanocomposite
6 of 14
on the surface of cotton fabric; (b) Structure of tannic acid.

4.2. IR Analysis
4.2. IR Analysis
The presence of functional groups on the modified cotton surface was confirmed
The presence of functional groups on the modified cotton surface was confirmed
through Fourier-transform infrared spectra. Figure 2 shows FTIR spectra of the unmodi-
through Fourier-transform infrared spectra. Figure 2 shows FTIR spectra of the unmodified
fied cotton (a), cotton fabric modified with the GPTMS–MWCNTs nanocomposite (b) and
cotton (a), cotton fabric modified with the GPTMS–MWCNTs nanocomposite (b) and
cotton fabric modified with MWCNTs–GPTMS-tannic nanocomposite (c). On account of
cotton fabric modified with MWCNTs–GPTMS-tannic nanocomposite (c). On account of
unmodified cotton fabric (a), a band appeared at 3200–3500 cm−1 − that was assigned to O–
unmodified cotton fabric (a), a band appeared at 3200–3500 cm 1 that was assigned to
H stretching. The bands in the range of 1500–800 cm−1 appeared − 1 as a result of the existence
O–H stretching. The bands in the range of 1500–800 cm appeared as a result of the
of C–H, O–H, C–O, and C–O–C vibrations, due to the cellulose [9]. Compared to blank
existence of C–H, O–H, C–O, and C–O–C vibrations, due to the cellulose [9]. Compared
cotton fabric, Figure 1b shows a weak signal around 770 cm−1 that −was assigned to the
to blank cotton fabric, Figure 1b shows a weak signal around 770 cm 1 that was assigned
stretching vibration of the Si-O-Si bonds, thus confirming that: (i)
to the stretching vibration of the Si-O-Si bonds, thus confirming that: (i) the the fabric wasfabric
modified
was
via a ring-opening
modified reaction between
via a ring-opening the GPTMS–MWCNTs
reaction between the GPTMS–MWCNTs nanocomposite and the and
nanocomposite cot-
ton fibers [36,37] and (ii) the –OH groups of the MWCNTs could
the cotton fibers [36,37] and (ii) the –OH groups of the MWCNTs could react only withreact only with the –
OCH3 groups of the GPTMS molecules. Additionally, two new
the –OCH3 groups of the GPTMS molecules. Additionally, two new bands appeared at bands appeared at 2910
and
29102857
and cm
2857that
−1
cm−were
1 thatrelated to the stretching
were related of the methylene
to the stretching groups from
of the methylene groupsthefrom
GPTMS the
molecules. Figure 2c shows the sharp peaks observed at 1706 and
GPTMS molecules. Figure 2c shows the sharp peaks observed at 1706 and 1604 cm−1were 1604 cm −1 that
that
attributed
were to thetostretching
attributed vibrations
the stretching of C=O
vibrations and aromatic
of C=O C=C, C=C,
and aromatic respectively, thus thus
respectively, con-
firming the adsorption of tannic acid onto the cotton-fabric surface
confirming the adsorption of tannic acid onto the cotton-fabric surface [15,38,39]. [15,38,39].

3300 2910 2857 1706 1604 770

110

100

90
c
80
Transmittance (a.u)

70 b
60

50 a
40

30

20

10

0
4000 3600 3200 2800 2400 2000 1600 1200 800 400

Wavenumber cm-1

Figure 2.
Figure FTIR spectra
2. FTIR spectra of
of the
the treated
treated fabrics.
fabrics. (a)
(a) Spectrum
Spectrum for
for blank
blank cotton
cotton (b)
(b) cotton
cotton fabric
fabric modified
modified
with GPTMS-MWCNTs
GPTMS-MWCNTsnanocomposite,
nanocomposite,and and(c)(c)cotton
cottonfabric
fabricmodified
modifiedwith
withMWCNTs-GPTMS-tannic
MWCNTs-GPTMS-tan-
nanocomposite.
nic nanocomposite.

4.3. SEM
4.3. SEM Analysis
Analysis
By conforming
By conformingthethedeposition
depositionofof
nanoparticles, SEM
nanoparticles, images
SEM are are
images usedused
to study the mor-
to study the
phology of the fabric surface [40]. Figure 3 illustrates SEM images of the untreated cotton
morphology of the fabric surface [40]. Figure 3 illustrates SEM images of the untreated
fabric (a), the MWCNTs–GPTMS-nanocomposite-treated cotton fabric (b), and MWCNTs–
GPTMS-tannic-acid-nanocomposite-treated fabric (c). The surface of the untreated cotton
fabric was clear and smooth (Figure 3a). In contrast, it is obvious that the sample treated
with MWCNTs–GPTMS in Figure 3b shows a coating layer of MWCNTs on the surface of
the fabric with some particulate agglomerations of carbon nanotubes. This confirms the
deposition of the MWCNTs–GPTMS nano-network structure. In addition, some crakes are
found on the surface of fibers because of the GPTMS-crosslinking effect. In comparison with
sample in (Figure 3c) that was treated with a uniform coating of the MWCNTs–GPTMS-
tannic acid nanocomposite. This could be due to the fact that the MWCNTs’ modification
by tannic acid could enhance the compatibility between GPTMS and the MWCNTs [15].
On the other hand, the elemental composition of the coated fabrics was confirmed using
EDX analysis. Figure 3e,f confirmed the deposition of MWCNTs, GPTMS and tannic onto
surface of the cotton fabric with respect to Figure 3d of the untreated fabric.
 effect. In comparison with sample in (Figure 3c) that was treated with a uniform coating
of the MWCNTs–GPTMS-tannic acid nanocomposite. This could be due to the fact that
the MWCNTs’ modification by tannic acid could enhance the compatibility between
GPTMS and the MWCNTs [15]. On the other hand, the elemental composition of the
coated fabrics was confirmed using EDX analysis. Figure 3e,f confirmed the deposition of
Coatings 2022, 12, 178 7 of 14
MWCNTs, GPTMS and tannic onto surface of the cotton fabric with respect to Figure3d
of the untreated fabric.

(a) (b) (c)

(d) (e) (f)

Figure
Figure 3.
3.SEM
SEMimages
imagesand
andEDX
EDXanalysis
analysisof
ofthe
thetreated
treatedand
anduntreated
untreated cotton
cotton fabric.
fabric. (a)
(a)SEM
SEMfor
forblank
blank
cotton (b) SEM for cotton fabric modified with GPTMS–MWCNTs nanocomposite, (c) SEM for cot-
cotton (b) SEM for cotton fabric modified with GPTMS–MWCNTs nanocomposite, (c) SEM for cotton
ton fabric modified with MWCNTs–GPTMS-tannic nanocomposite, (d) EDX for blank cot-ton, (e)
fabric modified with MWCNTs–GPTMS-tannic nanocomposite, (d) EDX for blank cot-ton, (e) EDX
EDX for cotton fabric modified with GPTMS–MWCNTs nanocomposite, and (f) EDX for cotton fab-
formodified
ric cotton fabric
withmodified with GPTMS–MWCNTs
MWCNTs–GPTMS-tannic nanocomposite, and (f) EDX for cotton fabric
nanocomposite.
modified with MWCNTs–GPTMS-tannic nanocomposite.
4.4. Antibacterial Activity
4.4. Antibacterial Activity
The
The antibacterial
antibacterial property
property of
of coated
coated fabrics
fabrics with
with different
different treatments
treatmentsincluding
includingcot-
cot-
ton/GPTMS, cotton/tannic acid, cotton/GPTMS/MWCNTs, cotton/GPTMS/MWCNTs
ton/GPTMS, cotton/tannic acid, cotton/GPTMS/MWCNTs, cotton/GPTMS/MWCNTs
then
then tannic
tannicacid,
acid,cotton/GPTMS/tannic
cotton/GPTMS/tannic acid/MWCNTs
acid/MWCNTs nanocomposites against
nanocomposites two well-
against two
well-known types bacteria was evaluated. Gram-positive (S. aureus and B. subtilis) and
Gram-negative (E. coli and P. aeruginosa) are broadly used as bio-detectors of pollution.
Table 1 summarizes the evidence of antibacterial activity. The antibacterial action in
the nanocomposites containing MWCNTs requires a closing to be attached between the
MWCNTs and the micro-organisms. An effective antibacterial character was observed
due to the presence of MWCNTs on the cotton surface. It is noteworthy that the highest
inhibition zones for S. aureus and E. coli were observed upon the post-treatment of the
MWCNTs–GPTMS-nanocomposite fabric with tannic acid (26 mm, 24 mm). Many studies
have indicated that MWCNTs allow for the capability of adhesion to micro-organisms;
subsequently, they can be utilized to eliminate a diverse array of biological pollutants,
involving bacteria, viruses, natural organic matters, and cyanobacterial toxins. This was
proposed because of their fibrous morphology, which encroaches upon the bacterial cell
surface and disturbs the intracellular metabolic pathways [26,41,42].
 rial character
indicate
bacterial
bacterial
bacterial the cells
cells ofdie.
cellsthe
durability
die. MWCNT-treated
of the treated
Furthermore,
die. Furthermore,
Furthermore, bacterial
bacterial
bacterial fabric
cotton
growth
growth
growth was
fabricis improved
towards
is restricted
is is restricted
restricted by
by bythe
repeated
the
by
the the presence
washing
presence
the presence
presence of
of tannic
of of tannic
cycles.
tannic
tannic The
rial It
treated is
character
rial noteworthy
bacterial
samples
bacterial
character of
cells die.
kept
cells
the of that
die. tannic
Furthermore,
their antibacterial
Furthermore,
MWCNT-treated
the MWCNT-treated acid
bacterial
bacterial
fabricplays
growth
properties
growth
was
fabric awasdualis
improved role
restricted
after 20by
restricted
improved in
by by the
the
washing
theby stabilization
presence
cycles.
presence
presence
the
ofof
presenceof
tannic
The
tannic
tannic
of of MW
antiba
aci
tanni
treated
acidIt
acid
acid
acid
acidasassamples
is
as noteworthy
it
itit prevents
as
as it
prevents
prevents
it kept
prevents
prevents the
thetheir
the that
the antibacterial
absorption
the tannicof
absorption
absorption
absorption
absorption ofacid
of sugar
of
sugar
sugar
of properties
plays
sugar
sugarand
and
andand
and aamino
aminoamino
amino
amino after
dual acids.
acids.20 The
role
acids.
acids.
acids. washing
The
Thein
The
The the
results
results
results cycles.
in
results
in
results Table
in
inin The
stabilization
Table
Table
Table
Table antibacte-
111 alsoof MW
11tannic
also
alsoalso
also
rial
and the character
Itrialimprovement
is noteworthy
It of
isimprovement
noteworthythe MWCNT-treated
of
that the
tannic
that functionalities
acid
tannic fabric
plays
acid was
awas
plays of
dual improved
the treated
role
atowards
dual in
role theby the
fabric presence
as well. of
These a
res
and indicate
indicate
character
indicate
the
indicate
indicate the
the
the the
thedurability
durability
ofdurability
the
durability
durability of
of
of
of the
of
MWCNT-treated
the the
the
the
of thetreated
treated
treated
treated
treated cotton
cotton
fabric
cotton
functionalities
cotton
cottonfabric
fabric
fabric oftowards
fabric
fabric towards
improved
the
towards
towards repeated
repeated
repeated
treated
repeated
repeatedthestabilization
byinfabricthe stabilization
washing
washing
presence
washing
washing
washing cycles.
cycles.
as well. of
cycles.
of
cycles.
cycles.The
tannic
The
These MWCNT
Theofacid.
The
The MW
resu
inand theIt
accordance
and
in
isIt noteworthy
treated
treated
improvement
the
treated
treated
treated
accordance
with
samples
samples
isimprovement
samples
noteworthy
samples
samples other
with
keptof
kept
kept
that
kept
kept the
their
that
their
other
tannic
previous
theirtheir
of
their
acid
antibacterial
antibacterial
tannic reports
antibacterial
functionalities
the acid
antibacterial
antibacterial
previous
playsofon
properties
functionalities
properties
plays
propertiesaa
properties
the
properties
reports on
dual
other
after
of treated
the
after
dual
after
after
other
role
20
after
20
role
20
inthe
materials
washing
20 washing
fabric
treated
washing
in
washing
20 washing
materials
the stabilization
as
fabric [15,44,45].
cycles.
cycles. The
cycles.
well.
cycles. as
cycles.The
stabilization
TheThe
These
well.
The
[15,44,45].
ofresults
antibacte-
antibacte-
These
antibacte-
of MWCNTs
antibacte-
antibacte-
MWCN
resua
and the
inandrial
rial
in accordance
rial improvement
character
rial
the
accordance
rial character
character withof
improvement
character
character of the
of
the
other
with
ofofthetheof the
MWCNT-treated
the
MWCNT-treated
of the
previous
other
MWCNT-treated functionalities
MWCNT-treated
MWCNT-treated fabric
fabric
functionalities
previous reportsfabric was
fabric
was
on
reportswas
fabric of
was
of
was the
improved
the
other
on
improved treated
improved
improved treated by
by
materials
other
improved fabric
the
by
the
fabric
materials
bybythe presence
the as
presence
presence well.
of
of
as[15,44,45].
well.
[15,44,45].
thepresence
presence These
ofof These
tannic
of tannic
tannic
tannic
tannicacid.
acid. results
acid.
results
acid. are
acid.
Coatings 2022, 12, 178 8 of 14
in accordance It
It
It is
It
is
is
It noteworthy
is noteworthy
with
noteworthy
noteworthy
is other
noteworthy that
that
that tannic
that
previous
that tannic
tannic
tannic
tannic acid
acid
acid
acid
acidplays
reports plays
plays
plays
playsa
on
aa dual
a
dual
dual
a dual
other
dual role
role
role in
role
in
rolein the
in
materials
the
the
in stabilization
the
the stabilization
[15,44,45].
stabilization
stabilization
stabilization of
of
of MWCNTs
of MWCNTs
MWCNTs
MWCNTs
of MWCNTs
TableTable1.
in Antibacterial
accordance
1. Antibacterial withactivity
other
activity andand
previous durability
reportsproperties.
durability on other materials [15,44,45].
properties.
and
and the
and improvement
thethe
improvement of
of the
improvement of functionalities
thethe
functionalities of
of the
functionalities of treated
thethe
treated fabric
treated
fabric as
fabric well.
as as
well. These
well.
These results
These results
results are
areare
TableTable1.and 1.the
and improvement
the
Antibacterial improvement
Antibacterial activity ofand
the
of
activity thefunctionalities
functionalities
durability
and durability ofproperties.
the
of
properties. treated
the treated fabric
fabricasas
well.
well. These
Theseresults
resultsareare
in
in
in accordance
in
in accordance
accordance
Inhibition
accordance
accordance with
with
with
with other
other
Zone
withother previous
other
other(mm previous
previous
previous per
previous reports
reports
reports
1reports
cm
reports on
on other
on
other
Sample)
on onother materials
other materials
materials
othermaterials
materials [15,44,45].
[15,44,45].
[15,44,45].
[15,44,45].
[15,44,45].
Table 1.
Table Antibacterial
1. Antibacterial
Inhibition activity
activity
Zone andand
(mm durability
durability
per
Table 1. Antibacterial activity and durability properties. 1 cmproperties.
properties.
Sample)
G+Table
TableG+Inhibition
Table1.
1.
Inhibition
Antibacterial
Antibacterial
Inhibition
ZoneZone
1. Antibacterial
Antibacterial
(mm (mm
activity
activity
Zone and
activity
and
(mm
per 1per cm 1Sample)
durability
and
durability
per
cm Sample)
cmproperties.
durability
1cm properties.
properties.
Sample)
G−
G−
Table
Table 1.Inhibition
Antibacterial
1. Zone
activity(mm
activityandand per 1
durability
durability Sample)
properties.
properties.
trate/Treatment of Fabric
Substrate/Treatment of Fabric G+ G+
S.G+aureus Inhibition
S. aureus Zone (mmB.(mm per 1
subtiliscm
B. subtilis Sample) E.E.coli
coli G− G− P.aeruginosa
P. aerugino
G+ Inhibition
Inhibition
Inhibition ZoneZone
Zone (mm
(mm per
per 111cm
per 1 cm
cm Sample)
cm Sample)
Sample) G−G−
ubstrate/Treatment
Substrate/Treatment of Fabric
of Fabric S. aureus
G+ S. Inhibition
aureusInhibition Zone B.
Zone (mm (mm per
subtilis
B. cm
subtilis
per 1 Sample)
Sample) E. coliE. coli G − P. aeruginosa
P. aeruginosa
No. No. of washing
cycleofcycle
of Substrate/Treatment
washing of Fabric1 1G+ 20 20
S. aureus
G+ 1 B.1B.subtilis
subtilis 2020 1 1 E.E.coli 20
20G− G− 11
P. aeruginosa 2020
Substrate/Treatment
No. of washing
No. of cycle
washing Fabric
cycle 1 S.G+
1 G+aureus
G+ 20 20 1 1 20 20 1 1 coli
20
G−
G−G−
20 1 P.
1 aeruginosa
20 20
Substrate/Treatment
No. of washing cycleof FabricFabric 1 S. S. aureus 0.0
20 1B.B. subtilis 200.0 1 E. E. coli
coli 20 0.00.0 P. aeruginosa
1aeruginosa
aeruginosa 20 0.0
No. ofSubstrate/Treatment
cycle of
Substrate/Treatment
Substrate/Treatment
Substrate/Treatment
Substrate/Treatment
washing ofFabric
of of
Fabric
Fabric
of Fabric
1 aureus
S.0.0
S. S. aureus
aureus
aureus
S. aureus
20 1 B.subtilis
B. B. subtilis
subtilis
subtilis
B. subtilis
20
0.0 1 E.coli
E. E.
coli
coli
E. coli 20 P.
P.aeruginosa
P. P.
aeruginosa
P. aeruginosa
1 20 0.
No.
No. of
No. of
No. washing
of
Washing
of washing cycle
washing
Cycle cycle
cycle 1 11 1 0.0 0.0
20
20
0.0 20 1
1 1 0.020
202020 0.0 1
1 1
1 20
20 0.0
0.0
20 0.0 1
1 1 1 20
20 20 0.0
0.0 0.0
No. ofof
No. washing
washingcycle
cycle 1 1 2020 1 1 20 20
0.0 1 1 2020 1 1 2020
cotton/GPTMS 0.00.0 0.0 0.0 0.0
cotton/GPTMS 0.0 0.0 0.0
0.00.0
0.0 0.0 0.0 0.0
0.0
0.0
0.0
0.00.0
0.0 0.00.0 0.00.0
0.00.0
0.0
0.0
0.0
0.0
0.0
0.0
0.0 0.0
0.0
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS 0.0 0.0 0.0 0.0 0.00.0 0.00.0 0.0 0.0 0.0
0.0
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS
cotton/GPTMS 0.0 0.00.0
0.00.0
0.00.0 0.0
0.0
0.0 0.0
0.00.0 0.0
0.0 0.0
0.0
0.0
0.00.0 0.0
0.0 0.0 0.0
0.0
0.00.0
15
20 23 19 1515 1515
20 20
20 20 23 23
23 23 19 19
19 19 15
15 15
1515
15
20
20 20 23
232323 19
19 19
1919 15
cotton/tannic acid 21 20 2020 26
23
2323 20 19 17
cotton/tannic
cotton/tannic
cotton/tannicacid
acid
cotton/tannic acid
acid acid 21
21 21 2121 26
262626 202020 17 17 17
cotton/tannic
cotton/tannic
cotton/tannicacid
cotton/tannic
acid
acid
cotton/tannic
cotton/tannic acid acid 2121 21
2121 2626
26
26 26 2020
20
20
20 20
20 17
17
17
1717 17 17
cotton/tannic acid 21 26 20 17

15
15
15
15 15 17
17171717 18
18 1818 18
1818
15
15
15
15 15
1515
15
15
1515 1717
17 18
18 18 15 1515
15 1717 17 18
Coatings 2022, 12, x FOR PEER REVIEW 15 15 17 18
915
of 14
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs 1616 16 15 20 20
2020 19 19 19 17 17 17
Coatings
Coatings
Coatings 2022,
2022,
2022,
Coatings
Coatings 12,
cotton/GPTMS/MWCNTs
2022, xxx12,
12,
12, FOR
xxFOR
FOR
cotton/GPTMS/MWCNTs
Coatings 2022,
2022,12,
12,
cotton/GPTMS/MWCNTs FOR PEER
PEER
PEER
x FOR
cotton/GPTMS/MWCNTs
FORPEER REVIEW
REVIEW
REVIEW
PEER
PEER 1616
16
REVIEW
REVIEW
REVIEW 1616 20
20
20 20 19 19
1919
19 171717 17
17 99999of
ofof
of 14
914
of1414
of
14 14
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs 16 16 20 20 19 19 17 17
tton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs 16 16 20
20 1919 17 17
25 21 23 22
25
2525
25 25
25 21
21
21
21 21
21
21 23
23
23
23
232323 22
22
22
2222
22 22
25
cotton/GPTMS/MWCNTs then
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs
cotton/GPTMS/MWCNTs then
then
then
then
then then26
then 22 24 23
tannic acid 26
26
2626
26 26
26 22
22
22
2222
22 22 24
24
24
24 24
2424 23
23
23
23 23
23
23
tannic
tannic
tannic
tannic acid
acid
acid
tannic
acid
tannic acid
tannic acid
acid

16
16
1616
16 16
16 1616 16
16
16
16
16 16
16 15
15
15
15
151515
15 17
17
1717 1717
17
17

tannic
tannictannic
tannic
tannic
tannic
tannic
tannic 18
18 17
17 16
16 18
18
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs
acid/cotton/GPTMS/MWCNTs 1818
18 18 18
18 17
17
1717 17
17 16
16
16 16
16
16 18
18 18
18
18 18
acid/cotton/GPTMS/MWCNTs

4.5.
4.5.
4.5. UV
4.5. UV
4.5.4.5.
UV
UV Protection
UVProtection
Protection
UV Properties
Properties
Properties
Protection
Protection
Protection Properties
Properties
Properties
4.5. UV Protection
It was Properties
also observed that the inhibition-zone diameter for B. subtilis and E. coli recorded
To
To
ToTo examine
examine
Toexamine
To
examineexamine
examine the
the
thethe UV-radiation-protection
UV-radiation-protection
theUV-radiation-protection
the UV-radiation-protection
UV-radiation-protection
UV-radiation-protection character
character
character
charactercharacter ofof
of
of the
ofthethe blank
blank
theblank
of
the the
blank fabrics
fabrics
fabrics
blank
fabricsfabrics and
and
and
and the
the
and the nano-
thenano-
the thenano-
nano- nano-
the highest
To value among
examine the the other treated samplescharacter
UV-radiation-protection (26 mm, 20
character mm). blank
of theSimilar
blank
fabrics
to and
phenolic
fabrics and
nano-
acid,
the nano-
composite-coated
composite-coated
composite-coated
composite-coated
composite-coated
composite-coated cellulosic
cellulosic
cellulosic
cellulosic
cellulosic
cellulosic fabrics,
fabrics,
fabrics,
fabrics,fabrics,
fabrics, the
the
thethe
the UPF
UPF
UPF
the
UPF
UPF UPF(ultraviolet-protection
(ultraviolet-protection
(ultraviolet-protection
(ultraviolet-protection
(ultraviolet-protection
(ultraviolet-protection factor)
factor)
factor)
factor)factor)
factor) values,
values,
values,
values, values,
values, which
which
which
which which
which
tannic acid may be cellulosic
composite-coated classified infabrics, the polyphonicthe UPF group. It has been extensively
(ultraviolet-protection factor) researched
values, which
are
are
are defined
defined
aredefined
are defined as
as as the
asthethe
as ultraviolet-light-transmittance
ultraviolet-light-transmittance
ultraviolet-light-transmittance
the ultraviolet-light-transmittance percentage,
percentage,
percentage,
percentage, were
were
were estimated
estimated
estimated
were estimated and
and and the
the
and the
there-re-
there-
re-re-
inare
are the defined
defined
biomedical
defined as
as the
the
the
fieldultraviolet-light-transmittance
ultraviolet-light-transmittance
as it has remarkable antiviral
ultraviolet-light-transmittance
percentage,
percentage,
and were
were
antibacterial
percentage,
estimated
were
estimated
properties.
estimated
andand the
Tannicand
re-
the re-
sults
sults
sults
sults are
are
are
sults outlined
outlined
outlined
are outlined in
in in Table
Table
Table
in Table 2.
2. 2. 2.
acid isare
sults areoutlined
active outlined
against ininTable
Table2.2.
Gram-positive and Gram-negative bacteria, while it also shows
sults are As
As
AsAs outlined
the
the
As
Asthe the
the table
thetable
table
table in
table
tableshows, Table
shows,
shows,
shows, shows,
shows, the
the2.
the
the
theUV UV
UV
theUV
UV resistance
UVresistance
resistance
resistance
resistance
resistance and
andand
and
andwash wash
wash
wash
and washdurability
durability
durability
washdurability durability
durability of
ofof the
thethe
of
ofofacid
the modified
modified
modified
the
themodified modified cotton
cotton
cotton
cotton cotton
outstanding biological properties. The antibacterial adequacy of tannic ismodified
disclosed cotton
by
fabrics
fabrics
fabrics
As
fabrics
fabrics were
thewere
were
fabricswere
werewere measured.
table measured.
measured.
measured.
measured.shows,
measured. The
The
The
Thethe
The treatment
treatment
treatment
The UV treatment
treatment resistance
treatment ofof
of
of ofcotton
cotton
cotton
of
cotton cotton
cotton and fabric
fabric
fabric
fabric with
fabric
wash
fabric with
with
with
with tannic
withtannic
tannic
durability
tannictannic
tannic acid
acid
acid
acidof
acid showed
acid
theshowed
showed
showed showed
showed modifiedaaaaagreat
great
great
a great
great
great cotton
its ability to penetrate the bacterial cell wall up to the inward layer, thereby obstructing
UV-protection
UV-protection
UV-protection
fabrics UV-protection factor
factor
factor estimated
estimated
estimated
factor estimated atat
at 96.2,
96.2,
96.2,
at which
which
which
96.2, which was
waswas additionally
additionally
additionally
was additionally improved
improved
improved
improved by
by by treatment
treatment
treatment
by treatment
the metamorphosis of the cell and inducing cell death. In Gram-positive bacteria, tannins great
were
UV-protection
UV-protection measured.
factor
factor The
estimated
estimated treatment
atat96.2,
96.2, of
which cotton
which was
was fabric
additionallywith
additionally tannic
improved
improved acid byby showed
treatment
treatment a
with
with
with
with
with
UV-protection MWCNTs.
MWCNTs.
MWCNTs.
with MWCNTs.
MWCNTs.
MWCNTs. The
The
The
factor The
The cotton
cotton
cotton
The
cotton cotton
cotton
estimated fabric
fabric
fabric
fabric
fabric treated
treated
treated
fabric
treated
atin treated
treated
96.2, with
with
with
with
with
which with GPTMS/MWCNTs
GPTMS/MWCNTs
GPTMS/MWCNTs
GPTMS/MWCNTs
GPTMS/MWCNTs
GPTMS/MWCNTs
was additionally then
then
then
then
thenthentannic
tannic
tannic
tannic
improved tannic
tannic acid
acid
acid
acid
acid
by dis-
aciddis-
dis-
dis-
dis-
treatmentdis-
are quickly dynamic. Nonetheless, Gram-negative bacteria, the process is slower on
played
played
played
played played aa a UV-protection
UV-protection
UV-protection
a UV-protection factor
factor
factor factor estimated
estimated
estimated
estimated up
upup to
to
up to 152.1.
152.1.
152.1.
to Tannic
Tannic
Tannic
152.1. Tannic acid
acid
acid afforded
afforded
afforded
acid afforded protection
protection
protection
protection
with played
account ofa athe
MWCNTs. UV-protection
UV-protection
The cotton
presence factor
of the factor estimated
fabric estimated
double-layer treated upupwith
membrane.toto152.1.
152.1. Tannic
GPTMS/MWCNTs
TannicTannic acid
acid acid afforded
preventsafforded
then protection
thetannic protection
bacteria acid dis-
against
against
against
againstagainst
against UV-B
UV-B
UV-B
UV-B
UV-BUV-B [46,47].
[46,47].
[46,47].[46,47].
[46,47].
[46,47]. “Dark”
“Dark”
“Dark”
“Dark” “Dark”
“Dark” colors
colors
colors
colors colors
colors (such
(such
(such
(such (such
(such as
as
asas
as dark
dark
as
darkdark
dark darkgreen,
green,
green,
green, green,
green, red,
red,
red,
red,
red, navy
navy
navy
red,
navy
navy blue,
navy blue,
blue,
blue, and
and
blue,
blue, and
andand andblack)
black)
black)
black) black)
black) offer
offer
offer
offer
offer offer
from binding
played to the surface factor
a UV-protection [43]. When estimatedbacteriaup do not adhere Tannic
to 152.1. to the surface, bacterial cells
acid afforded protection
greater
greater
greater
greater
die. greater
greater protection
protection
protection
protection
protection
Furthermore,protection than
than
than
than
than
bacterial “light”
“light”
“light”
than
“light”“light”
“light”
growth colors.
colors.
colors.
is colors.
colors.
colors. Treatment
Treatment
Treatment
Treatment
Treatment
restrictedTreatment
by dark the with
with
with
with
with MWCNTs
withMWCNTs
MWCNTs
MWCNTs MWCNTs
MWCNTs
presence of endows
endows
endows
endows
tannic endows
endowsacid the
the
the
asthe
the black
theblack
itblack
black
blackblack
prevents color
color
color
color
colorcolor
against
to
toto cotton
cotton
to
UV-B
cotton
cotton
[46,47].
fabric,
fabric,
fabric, which
which
which
fabric,
“Dark”
which provides
provides
provides
provides
colorsexcellent
(such
excellent
excellent
excellent UV
as
UV
UV protection.
protection.
UV
green,
protection.
protection.
red,
This
This
This may
This
navy
may
may may be
bebe
blue,
the
thethe
be
and
result
result
result
the result
black)
of
of of the
thethe
of
offer
the
to
the to cotton
cotton
absorption fabric,
fabric,
of which
sugarwhich and provides
provides
amino excellent
excellent
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and
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more uniform
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dispersal
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absorb
absorb
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absorbof visible
visible
visible
visible
visible light
light
light
visible
Furthermore, light [17].
[17].
[17].
light
[17].
light [17].
the functionalities it [17].
was found that the optical behavior
of the treated fabric as well. These results are in of the MWCNTs is
due to theirwith
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other previous andreports
alignment. Aligned
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[15,44,45].
Table
Table
Table 2.2.
2.
Table
Table
Table2.2.UPF
UPF
UPF values
values
values
2. UPF
UPF
UPF ofof
of
values
values
valuesof cotton
cotton
ofcotton fabrics
fabrics
fabrics
of cotton
cotton
cotton treated
treated
treated
fabrics
fabrics
fabrics under
under
under
treated
treated
treated different
different
different
under
under
underdifferent
different conditions.
conditions.
conditions.
different conditions.
conditions.
conditions.
strongly absorb visible light [17].
Treatment
Treatment
Treatment
Treatment
Treatment
Treatment UPF
UPF
UPF
UPF
UPF Value
UPFValue
Value
ValueValue
Value UV
UVUV Protection
Protection
UVProtection
UV UV Protection
Protection
Protection
Table 2. UPF values of cotton
Blank
Blank
Blank fabrics treated under different
Blank
Blank
Blank 7.17.17.1conditions.
7.1
7.1
7.1 55555 5 Non-ratable
Non-ratable
Non-ratable
Non-ratable
Non-ratable
Non-ratable
Cotton/GPTMS
Cotton/GPTMS
Cotton/GPTMS
Cotton/GPTMS
Cotton/GPTMS
Cotton/GPTMS 6.8
6.8
6.8
6.8
6.86.8 55555 5 Non-ratable
Non-ratable
Non-ratable
Non-ratable
Non-ratable
Non-ratable
Treatmentacid
Cotton/tannic
UPF
96.2
Value 50+ UV Protection
Excellent
Cotton/tannic
Cotton/tannic
Cotton/tannic acid
acid
Cotton/tannic
Cotton/tannicacid acid
acid 96.2
96.2
96.2 96.2
96.2 50+
50+50+
50+ 50+ Excellent
Excellent
Excellent
Excellent
Excellent
Blank 7.1 5 Non-ratable
Coatings 2022, 12, 178 9 of 14

4.5. UV Protection Properties

To examine the UV-radiation-protection character of the blank fabrics and the
nanocomposite-coated cellulosic fabrics, the UPF (ultraviolet-protection factor) values,
which are defined as the ultraviolet-light-transmittance percentage, were estimated and the
results are outlined in Table 2.

Table 2. UPF values of cotton fabrics treated under different conditions.

Treatment UPF Value UV Protection

Blank 7.1 5 Non-ratable
Cotton/GPTMS 6.8 5 Non-ratable
Cotton/tannic acid 96.2 50+ Excellent
Cotton/GPTMS/MWCNTs 73.6 50+ Excellent
Cotton/GPTMS/MWCNTs then tannic acid 152.1 50+ Excellent
Tannic acid/cotton/GPTMS/MWCNTs 75.3 50+ Excellent

As the table shows, the UV resistance and wash durability of the modified cotton
fabrics were measured. The treatment of cotton fabric with tannic acid showed a great
UV-protection factor estimated at 96.2, which was additionally improved by treatment with
MWCNTs. The cotton fabric treated with GPTMS/MWCNTs then tannic acid displayed
a UV-protection factor estimated up to 152.1. Tannic acid afforded protection against
UV-B [46,47]. “Dark” colors (such as dark green, red, navy blue, and black) offer greater
protection than “light” colors. Treatment with MWCNTs endows the black color to cotton
fabric, which provides excellent UV protection. This may be the result of the black color
absorbing the radiation and altering the transmitting effect. Thanks to the post-treatment
with tannic acid, a higher load and a more uniform dispersal of the MWCNTs were
obtained. Furthermore, it was found that the optical behavior of the MWCNTs is due to
their homogeneity and alignment. Aligned nanotube networks can brief rate and strongly
absorb visible light [17].

4.6. Analysis of Conductivity

Table 3 shows the measurement of the electric properties of the MWCNT-based cotton-
fabric hybrids. The resistivity relative to the different treatments was recorded. However, he
introduced results show a conspicuous contrast in the sorption of the nanotube suspension
by the treated textile. Furthermore, the measurement of carbon nanotubes deposited onto
the surface of the cotton samples was generally influenced by the formulation. The increase
in electrical conductivity followed the order cotton/GPTMS/tannic acid/MWCNTs >
cotton/GPTMS/MWCNTs > cotton/GPTMS/MWCNTs then tannic acid > cotton/GPTMS
> cotton/tannic acid.

Table 3. Electrical properties of untreated and treated cotton fabric.

Treatment Resistivity Ω/cm

Untreated 245
Cotton/GPTMS 148
Cotton/tannic acid 150
Tannic acid/cotton/GPTMS/MWCNTs 115
Cotton/GPTMS/MWCNTs 120
Cotton/GPTMS/MWCNTs then tannic acid 145

In the case of the cotton-based (cotton/MWCNTs) hybrid materials, particularly those

with coatings, a large amount of the nanotube suspension defused and then stilled inside
Coatings 2022, 12, 178 10 of 14

the fiber structure, which affected the fiber conductivity. When GPTMS was present, it acted
as a network for the homogeneous distribution of CNTs on the fabric surface. The surface
deposition of MWCNTs was increased by this. The MWCNTs deposition was accompanied
by an improvement in the thickness of the surface layer. This directly contributed to
a decrease in the threshold for percolation and an increase in the surface conductivity.
Therefore, as a result of decreasing electrical resistivity, the surface electrical conductivity
increased; in the meantime, the tannic-acid adsorption allowed the nanotube suspension to
effectively penetrate the surface of the cotton fibers, infiltrating their porous construction
and leading to a highly conductive fabric structure. While the adsorption of the layers of
tannic acid onto the surface led to a lower effect of the MWCNTs, the fabric conductivity
was determined to be smaller than in the other treatments, and the conductivity of such
a composite was relatively low. The above outcomes show potential for controlling the
permeation edge and conductivity esteems of hybrid materials simply by applying carbon
nanotubes not only to the surface but also within the material.

4.7. Mechanical Properties

There are few reports of the impact of MWCNT deposition on cellulosic fabric’s me-
chanical characteristics [48]. Table 4 shows the roughness and tensile strength of the coated
surface of the cotton fabric. Table 4 clearly shows the improvement in tensile strength and a
slight increase in roughness values for the fabric treated either by MWCNTs–GPTMS or by
tannic-MWCNTs–GPTMS nanocomposites compared to the untreated fabric. This proves
the homogeneous coating of MWCNTs on the surface of the fabric and could be explained
by the strengthening effect of the carbon nanotubes dispersed in the nanocomposite [49]. In
addition, the mechanical properties of the polymer-microscalized fibers were significantly
improved by using nanomaterials such as carbon nanotubes as fillers or reinforcements
in composite materials. Moreover, the modified CNTs formed nanoscale surface rough-
ness on the microscale cellulose fabric, resulting in the formation of an artificial lotus-leaf
structure on the cotton [48]. On the other hand, samples treated with only GPTMS or with
tannic acid exhibited a decrease in tensile strength as well as an improvement in roughness
values compared with the untreated samples. This could be attributed to the effect of
the ether crosslinking or the acidity of the crosslinking agent’s cellulose structure leading
to a degradation of the cellulose polymer chains, thereby resulting in the reduction of
tensile strength.
Our results were compared to other reported results that indicate a negative impact
of using carboxylic acid as a crosslinking agent on tensile strength. The results in Table 4
demonstrate the importance of using GPTMS/tannic acid in the finishing formulation in
a certain sequence in order to enhance the performance of the MWCNT-treated cotton
fabric without affecting the physical properties [17]. Finally, Table 5 shows a comparative
study between the results of our work and previous work indicating, the importance of
using tannic acid as we as GPTMS in the finishing formulation with MWCNTs to improve
fabric performance.

Table 4. Tensile strength and roughness of treated and untreated cotton fabric.

Tensile Strength Roughness

Treatment
(Kg f) (µm)
Untreated cotton fabric 55 ± 0.86 14.5 ± 0.41
Cotton-GPTMS 46 ± 0.76 12.3 ± 0.37
Cotton-tannic acid 52 ± 1.50 12.7 ± 0.25
Cotton-GPTMS-MWCNTs 78 ± 0.36 15.4 ± 0.35
Cotton-GPTMS–MWCNTs drying then tannic acid 75 ± 0.5 14.9 ± 0.26
Tannic acid-cotton-GPTMS–MWCNTs 72 ± 0.65 15 ± 0.21
Coatings 2022, 12, 178 11 of 14

Table 5. Comparison between previous work and our work.

Previous Work Our Work

Treatment Functionalities Treatment Functionalities
-The abrasion resistance and UV
blocking capability are
Cotton fabrics were treated with nano improved,
titanium dioxide and multiwalled - tensile strength decreases
carbon nanotubes (MWCNTs) using -significant influence on the
succinic acid as a crosslinking self-cleaning properties of the
agent [26] treated cotton
fabricsparticularly when
exposed to sunlight Treatment of cotton
-Durable superhydrophobicity, fabric in Presence of Extra antibacterial, UV
A dip–dry–cure finishing process was ecofriendly tannic acid
-self-cleaning and flame protection, improvement
used to coat cotton fabric with as well as GPTMS is the
retardancy in tensile strength,
MWCNTs functionalized with mean key role in
-improved mechanical electrical conductivity
poly(butylacrylate) [48]. improvement of
resistance and UV protection
functions
Coating of MWCNTs onto cotton by
hydrophobicity to the fabric,
ultrasonic irradiation followed by the
this property was not durable
dipping method [24]
MWCNTs were coated with
tetraethylorthosilicate and a
fluoroalkoxysilane after being
Hydrophobicity and improved
noncovalently functionalized with an
conductivity
organic–inorganic hybrid consisting of
silica and an amphiphilic copolymer of
styrene and maleic anhydride [50].
The exhaustion method was used to
coat carbon nanotubes (CNTs) and fix
Increase the thermal stability of
them on a cotton surface utilising
the substrate.
1,2,3,4-butanetetracarboxylic acid
(BTCA) as a crosslinking agent [17]
A dyeing-like method was used to
Superhydrophobic behavior,
successfully incorporate MWCNTs into
flame-retardant
cotton and polyester substrates [51].
High-efficient flame retardant
MWCNTs were stabilized on a cotton
finishing of cotton fabrics and
surface using vinylphosphonic acid via
improvement of its thermal
UV irradiation [52]
properties.
(BTCA) and ZnO-BTCA-carbon
nanotube (CNT) composites were
Very good antibacterial activity
fabricated and coated on cotton fabric
by pad-dry-cure [53]

5. Conclusions
Cotton fabric was treated with a high-performance MWCNTs–GPTMS nanocomposite.
Tannic acid was added to the finishing formulation in different sequences to enhance the
sustainable functionalities of the treated fabric. GPTMS had no effect on the biological
activity of the treated cotton fabric. There was an improvement in tensile strength and a
slight increase in roughness values for the fabric treated either by MWCNTs–GPTMS or
by tannic-MWCNTs–GPTMS nanocomposites compared to untreated fabric. Outstand-
ing antibacterial properties were recorded in all the other treated fabrics while superior
properties were achieved upon the post-treatment with tannic acid for both S. aureus and
E. coli, i.e., large inhibition-zone diameters (26 mm, 24 mm). The post-treatment of cot-
ton/GPTMS/MWCNTs with tannic acid afforded a maximum UV-protection factor value
Coatings 2022, 12, 178 12 of 14

of 152.1. Modification with carbon nanotubes imparted high electrical conductivity only
in the case of pretreatment with tannic acid, which had the lowest recorded resistivity
value of 115 Ω/cm, while post-treatment with tannic acid negatively affected the electrical
conductivity and resulted in the high electrical-resistivity value of 145 Ω/cm.

Author Contributions: Conceptualization, M.M.A.E.-H. and A.F.; methodology, M.M.A.E.-H., A.F.

and S.S.; software, M.M.A.E.-H., S.S. and A.F.; validation, M.M.A.E.-H.; formal analysis, M.M.A.E.-H.
and S.S.; investigation, M.M.A.E.-H., A.F. and S.S.; resources, M.M.A.E.-H.; data curation, M.M.A.E.-H.
and A.F.; writing—original draft preparation, M.M.A.E.-H. and S.S.; writing—review and editing,
M.M.A.E.-H., A.F. and S.S.; visualization, M.M.A.E.-H.; supervision, M.M.A.E.-H., A.F. and S.S.;
funding acquisition, M.M.A.E.-H. and S.S. All authors have read and agreed to the published version
of the manuscript.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The data presented in this study are available on request from the
corresponding author.
Conflicts of Interest: The authors declare no conflict of interest.

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