coatings

Article
Development of Durable Antibacterial Textile Fabrics
for Potential Application in Healthcare Environment
Wen-Yi Wang 1 , Jia-Chi Chiou 2 , Joanne Yip 1 , Ka-Fu Yung 2 and Chi-Wai Kan 1, *
1 Institute of Textiles and Clothing, The Hong Kong Polytechnic University, Hung Hom, Kowloon,
Hong Kong, China; [email protected] (W.-Y.W.); [email protected] (J.Y.)
2 Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom,
Kowloon, Hong Kong, China; [email protected] (J.-C.C.); [email protected] (K.-F.Y.)
* Correspondence: [email protected]; Tel.: +852-2766-6531




Received: 17 April 2020; Accepted: 27 May 2020; Published: 29 May 2020


Abstract: Recently, efforts at development of functional textiles with antibacterial effect have accelerated,
the purpose being to provide protection against airborne bio-particles and micro-organisms. Growth of
microbes on surface of textile materials can be inhibited by biocidal approach and biostatic
approach. This paper describes the development of a healthcare textile with durable antibacterial
properties by optimizing the conventional and commercialized antimicrobial agent polybiguanide
derivative—poly(hexamethylenebiguanide) (PHMB). Pad-dry-cure method was used to coat PHMB
on cotton fabrics. The durability to simulated healthcare laundering of the fabric samples was
evaluated in detail. Specifically, effects of detergent and washing cycles were examined. It was found
that the optimum finishing condition can impart to the fabrics excellent durability for simulated
healthcare washing. The fabric samples showed 100% bactericidal effect after 52 washing cycles,
and 104 washings slightly reduced the bactericidal activity. Nevertheless, both simulated healthcare
washing and coating treatment were found to have slightly negative influence on the hand feel and
tearing strength properties of cotton fabrics.

Keywords: healthcare textile; antibacterial property; hand feel value; washing durability

1. Introduction
Cotton is a green natural cellulosic fiber available abundantly. It has been widely used in
daily life because of its favorable properties that include high strength, soft handle, affinity to skin,
and bio-degradability [1,2]. However, due to the morphology and moisture affinity of natural
origin, cotton fabrics provide a perfect environment for growth of microorganism on the surface [3].
Depending on moisture, nutrients, temperature and pH value, the bacterial growth can be very fast,
which may cause some undesirable effects, such as unpleasant odor, reduction of mechanical strength,
stains, and discoloration [1,4]. Even mild bacterial growth can lead to rotting and breakdown of the
fibers, which may make the fabric unattractive due to the appearance of unwanted pigmentation.
Moreover, the microorganism’s growth can accelerate the hydrolysis of cellulose and cause deterioration
of the fabric.
Microorganisms that frequently contaminate surface of cotton fabrics include Escherichia coli,
Klebsiella pneumoniae, Pseudomonas aeruginosa, Staphylococcus aureus, and Acinetobacter baumannii.
These can cause pathogenic effects on human beings due to user contamination and cross infection [5,6].
Therefore, it is of great concern for the textile industry to develop antibacterial textiles. The demand for
antibacterial textiles has been gaining increasing attention in the past few decades [7,8]. In healthcare
environment, textiles with antibacterial properties form a significant part of the hygienic regime
of surgical procedures, preventing the spread of infectious pathogens to both patients and staff.

Coatings 2020, 10, 520; doi:10.3390/coatings10060520 www.mdpi.com/journal/coatings

Coatings2020,
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2020,10, x FOR PEER REVIEW 22 of
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hygienic regime of surgical procedures, preventing the spread of infectious pathogens to both
patients and finishing
Antibacterial staff. Antibacterial finishingcarried
is thus typically is thusout typically
to givecarried
textilesout to give resilience
improved textiles improved
against
resilience against microorganisms to prevent destruction of fibers and discoloration, and increased
microorganisms to prevent destruction of fibers and discoloration, and increased durability of the
durability
textiles withoflonger
the textiles
life, whichwith plays
longer anlife, which role
important playsinan important
addressing role ininaddressing
hygiene clinical andhygiene
sensitive in
clinical and sensitive environments by minimizing microbial colonization of textiles and the potential
environments by minimizing microbial colonization of textiles and the potential for transfer from fabric
for transfer
surfaces from fabric surfaces [9–11].
[9–11].
In this context, numerous
In this context, numerous methods methods have have beenbeen developed
developed to to impart
impart antibacterial
antibacterial properties
properties to to
textiles to reduce the spread of microorganisms by killing or inhibiting their growth on the
textiles to reduce the spread of microorganisms by killing or inhibiting their growth on the fabric fabric
surface,
surface,
e.g., e.g.,modification
surface surface modification and finishing
and finishing [3,12]. Gao [3,12].
andGao and Cranston
Cranston reviewedreviewed the application
the application of various of
various antibacterial agents to impart textiles with antimicrobial functions [3]. For examples, the
antibacterial agents to impart textiles with antimicrobial functions [3]. For examples, the conventional
conventional
exhaust, exhaust,
pad-dry-cure pad-dry-cure
processes, sprayingprocesses, sprayingmethod
and foam finishing and foam finishing
have been method
extensively haveforbeen
studied the
extensively studied
antimicrobial finishingfor the antimicrobial
on textiles with triclosanfinishing on textiles
and silicon-based with triclosan
quaternary and silicon-based
agents [13,14]. Meanwhile,
quaternary agents [13,14]. Meanwhile, use of a wide variety of antibacterial agents in fabric finishing
use of a wide variety of antibacterial agents in fabric finishing has been widely investigated, ranging from
has been widely investigated, ranging from synthetic organic compounds, such as quaternary
synthetic organic compounds, such as quaternary ammonium salt [9,15], polybiguanides [16,17],
ammonium
and N-halamines salt [9,15], polybiguanides
[18], through to TiO2 , ZnO,[16,17],andandsilverN-halamines
nanoparticles [18], through
[6,10,19] andtonaturally
TiO2, ZnO, derivedand
silver nanoparticles [6,10,19] and naturally derived antimicrobials, such as chitosan [20]. Recently,
antimicrobials, such as chitosan [20]. Recently, the combination of antibacterial and hydrophobicity for
the combination
cotton of antibacterial
fabric has attracted and hydrophobicity
much interest for cotton
for better antibacterial fabric has
behavior. Forattracted
example,much Mohammadinterestand for
better antibacterial behavior. For example, Mohammad and colleagues developed such a dual-
colleagues developed such a dual-functional antibacterial textile by immobilizing silver nanoparticles
functional
as antibacterial
the antibacterial agent textile
and by thenimmobilizing
modified itsilver with nanoparticles
octyltriethoxysilane as the (OTES)
antibacterial agent and
to achieve the
then modified
hydrophobic it with
surface [21].octyltriethoxysilane
Thirumalaisamy et(OTES) to achieve
al. explored the method the hydrophobic
of bimetallicsurface
deposition [21].
Thirumalaisamy et al. explored the method of bimetallic deposition to obtain superhydrophobic and
to obtain superhydrophobic and antibacterial cotton fabric [22]. Recently, some novel methods
antibacterial
of antibacterial cotton fabrichave
finishing [22]. been
Recently, some novel
reported. In thismethods
regard, Poonamof antibacterial finishing fabricated
and coworkers have been
areported. In this regard, Poonam and coworkers fabricated a dual-functional cotton fabric
dual-functional cotton fabric with superhydrophobicity and antibacterial property by with
simply
superhydrophobicity and antibacterial property by simply immersing cotton fabric in non-
immersing cotton fabric in non-fluorinated hexadecyltrimethoxysilane solution [23]. The modified
fluorinated
cotton fabrichexadecyltrimethoxysilane
not only shows excellent antibacterial solution [23].property,The modified but also cotton has fabric not only
outstanding shows
oil-water
excellent antibacterial property, but also has outstanding oil-water separation efficiency. Another
separation efficiency. Another example is the environmentally friendly antibacterial cotton fabric
example is the environmentally friendly antibacterial cotton fabric reported by Chen et al. [24], which
reported by Chen et al. [24], which was finished with siloxane sulfopropylbetaine (SSPB). SSPB was
was finished
found not to be with siloxane
leachable fromsulfopropylbetaine
the fabric and the(SSPB). SSPB was
coated fabric found not
is nontoxic to beRong
to skin. leachable from the
et al. reported
fabric and the coated fabric is nontoxic to skin. Rong et al. reported the method of heterogeneous
the method of heterogeneous transesterification to develop hydrophobic and antibacterial cotton
transesterification
fabric via constructing to develop
enaminehydrophobic
bonds between andacetoacetyl
antibacterial cotton
groups and fabric
cotton viafiber
constructing enamine
[1]. The resulting
bonds between acetoacetyl groups and cotton fiber [1]. The resulting material showed excellent
material showed excellent and durable bacteria-resistance rates of over 99.99% against E. and
coli and
durable bacteria-resistance rates of over 99.99% against E. coli and S. aureus. Additionally, novel
S. aureus. Additionally, novel graphene oxide based antibacterial cotton fabric has also been reported
graphene
and oxide based
extensively antibacterial
investigated by Zhao cotton
andfabric has also been
his colleagues [25].reported
However, andalthough
extensively investigated
these attempts
by Zhao and his colleagues [25]. However, although these attempts are highly meaningful and of
are highly meaningful and of importance for academia, there are still a long way from large-scale
importance
industrial for academia, there are still a long way from large-scale industrial production.
production.
Polyhexamethylene biguanide
Polyhexamethylene biguanide (PHMB)(PHMB)isisaawidely widelyused usedpolymeric
polymericantibacterial
antibacterial agent
agentdue dueto to
its
low toxicity and broad-spectrum biocide property, which has been commercially available in the
its low toxicity and broad-spectrum biocide property, which has been commercially available in the
market [15,26].
market [15,26]. It It is
is usually
usually used used asas aa biocide,
biocide, and and is is also
also an
an important
important drug drug usedused inin several
several topical
topical
applications. PHMB is composed of repeated basic biguanidine units connected by hexamethylene
applications. PHMB is composed of repeated basic biguanidine units connected by hexamethylene
hydrocarbon chains,
hydrocarbon chains, providing
providing aa cationic
cationic and and amphipathic
amphipathic structure
structure (Figure(Figure1). 1). The
The antibacterial
antibacterial
activityofof
activity PHMBPHMB dependsdepends on theon the molecular
molecular structure,structure,
which increaseswhichwith increases
the levelwith the level of
of polymerization,
polymerization,
and the maximum andbiocidal
the maximum efficiency biocidal
is obtainedefficiency
when is obtained when the hexamethylene
the hexamethylene group is employed groupas is
employed as the spacer [16]. Biguanides in the PHMB molecules account for the inhibition and
the spacer [16]. Biguanides in the PHMB molecules account for the inhibition and binding activities
binding
of PHMB.activities of PHMB.

Figure 1.
Figure 1. Chemical
Chemical structure
structure of
of poly(hexamethylenebiguanide)
poly(hexamethylenebiguanide) (PHMB).
(PHMB).
Coatings 2020, 10, 520 3 of 13

However, a major concern for PHMB coating on fabric surface consists in the compromised tearing
strength and hand feel values. The present study is thus focusing not only on the antibacterial behavior
and durability, but also on the physical properties of cotton fiber after coating with PHMB formulation.
The resulting cotton fabrics were subjected to detailed characterization by using a series of analytical
techniques, including hand feel measurement and tearing strength.

2. Materials and Methods

2.1. Materials
One hundred percentwoven cotton fabric (fabric weight 272.8 g/cm2) was used in this study. Originally,
the fabric was scoured in an aqueous solution containing 5 g/L sodium hydroxide (chemical grade, obtained
from Sigma-Aldrich, St. Louis, MO, USA) to remove impurities at temperature of 60 ◦C for 30 min,
after which it was thoroughly rinsed with tap water and dried at room temperature.
Antibacterial agent PHMB (20% w/v aqueous solution), PEG400 (400 g/mol in average) and
polyurethane binder (20% w/v aqueous solution) were supplied by Breakthrough Textiles Co., LTD.
(Taipei, Taiwan). The commercial detergent (Attack, concentrated liquid, 3 L, Kao (HK) Corp.,
Tokyo, Japan) was obtained from a local supermarket. Non-ionic detergent, C13 Oxoalcoholethoxylate
(7EO), was obtained from SDC Enterprises Limited, Holmfirth, UK. Sodium hypochlorite (NaClO) and
bromophenol blue (BPB) sodium were obtained from Sigma-Aldrich (St. Louis, MO, USA).

2.2. Pad-Dry-Cure Treatment

Finishing formulations were prepared by adding different amounts of PHMB, PEG400, and binder
to deionized water, and the “pad-dry-cure” method was used to coat the antibacterial agent on the
cotton fabric. Specifically, the fabric sample was first padded with finishing formulations with 80% wet
pickup and then dried in thermal oven (Werner Mathis AG, Switzerland) at 90 ◦ C for 5 min and cured
in Mathis LabDryer (Werner Mathis AG, Switzerland) at 130 ◦ C for 45 s with fan speed of 1600 rpm.
After antibacterial finishing, fabric samples were stored under standard conditions at 20 ± 2 temperature
and 65 ± 2% relative humidity for at least 24 h prior to subsequent testing.

2.3. Washing Test

Washing test was conducted to evaluate effects of simulated healthcare laundering on antibacterial
property of coated fabric samples. Different washing conditions with three washing cycles (26/52/104)
were used (Table 1). The test was conducted in a laboratory scale washing machine (Launder-Ometer,
SDL Atlas, Rock Hill, SC, USA). After each washing cycle, the fabric sample was withdrawn and
washed with tap water, and then the same volume of washing bath was added for the next cycle.
Bleaching agent sodium hypochlorite (NaClO) was used in the washing solution.

Table 1. Washing test conditions 3 .

No Detergent With Detergent

0 1
Solution 1 1 S10 S11
Solution 2 2 S20 S21
1 Solution 1: 75 ◦ C, 5 min, with or without detergent; 2 Solution 2: 65 ◦ C, 10 min + NaClO (300 ppm), with or
without detergent; 3 Washing cycles: 26/52/104.

2.4. Antibacterial Property

Antibacterial property of treated samples was qualitatively investigated against gram-positive
S. aureus and gram-negative K. pneumoniae according to AATCC TM 147-2011, and the quantitative
determination was performed in accordance with AATCC TM100-2019. The bacteria was grown
Coatings 2020, 10, 520 4 of 13

in nutrient agar at 37 ◦ C for 18 h. Fabric samples were cut into 20 mm × 20 mm pieces for the
antibacterial test.

2.5. Scanning Electron Microscopy (SEM) Observation

Surface morphology of the fabric samples was observed by SEM (JEOL Model JSM-6490,
JEOL USA, Inc., Peabody, MA, USA) with imaging up to 300,000× with a high resolution of 3 nm.
The samples were treated by spray-gold prior to observation.

2.6. Qualitative Determination of PHMB by Dyeing with BPB

The anion of the aqueous sodium salt of BPB can be complexed with the cationic polymers on
a substrate, leading to formation of a blue stable complex, which provides a standard method to
determine cationic polymers [27,28]. The present study utilizes BPB to qualitatively determine the
presence of PHMB coated on the fabrics.

2.7. Fourier Transform Infrared Spectroscopy Analysis

The physiochemical properties of PHMB-coated cotton fabric were analyzed via Fourier transform
infrared spectroscopy (FTIR, Spectrum 100 FT-IR Spectrometer, Perkin Elmer, Waltham, MA, USA).
The fabric samples were fastened on the sample stage and scanned from 400 cm−1 to 4000 cm−1 with a
resolution of 4 cm−1 .

2.8. Tearing Strength Analysis

Tearing strength of fabric samples before and after PHMB coating was measured by Elmendorf
Tear Strength Tester according to American Society for Testing and Materials (ASTM) D2261 standard.
Three specimens (200 mm × 75 mm) were measured for each sample.

2.9. Hand Feel Measurement

The hand feel value was analyzed by the PhabrOmeter instrument (Nu Cybertec, Inc., Davis, CA, USA)
according to AATCC Test Method 202-2014. For the purpose of discussion, hand feel index (HFI) is
defined as summation of resilience, softness, and smoothness, as shown in Equation (1).

HFI = Resilience + Softness + Smoothness. (1)

3. Results

3.1. Surface Morphology

Optical photographs and SEM were performed to observe the change in surface morphology of
the fabric samples after coating with PHMB formulation. Clearly, the surface of cotton fabric was
smooth (Figure 2A). From Figure 2B, the coated PHMB was obviously observed, and BPB dyeing
confirms that antibacterial agent PHMB was successfully coated on the surface of the cotton fabric
(Figure 2D).

3.2. FTIR Measuremnt

FTIR analysis was conducted to confirm the presence of PHMB on the treated cotton fabric,
as shown in Figure 3. A sharp and strong absorbance peak at 1550 cm−1 was observed in the spectrum of
PHMB, characteristic of imine group. The broad double peaks at 3195 cm−1 and 3380 cm−1 are ascribed
to stretching vibration of –NH- and –NH2 - of PHMB molecule. Compared to PHMB, the absorption
spectrum of cellulose is pretty weak, particularly for the untreated control cotton fabric. As shown in
the insert, the characteristic peak of cellulose at 3330 cm−1 becomes stronger after coating with PHMB,
which demonstrates that PHMB was successfully coated on the cotton fabric.
Coatings 2020, 10, 520 5 of 13

Coatings 2020, 10, x FOR PEER REVIEW 5 of 13

Figure 2. Surface morphology of treated fabric observed by SEM: (A) untreated cotton fabric, (B)
fabric treated with PHMB, and optical photographs: (C) untreated cotton fabric and (D) PHMB-coated
fabric dyed with bromophenol blue (BPB).

3.2. FTIR Measuremnt

FTIR analysis was conducted to confirm the presence of PHMB on the treated cotton fabric, as
shown in Figure 3. A sharp and strong absorbance peak at 1550 cm−1 was observed in the spectrum
of PHMB, characteristic of imine group. The broad double peaks at 3195 cm−1 and 3380 cm−1 are
ascribed to stretching vibration of –NH- and –NH2- of PHMB molecule. Compared to PHMB, the
Figure 2.
absorption Surface morphology
spectrum of cellulose of
is treated fabric observed
pretty weak, by SEM:
particularly (A)untreated
for the untreated control
cotton fabric,
cotton(B)
fabric.
Figure 2. Surface morphology of treated fabric observed by SEM: (A) untreated cotton fabric, (B) fabric
fabric treated
As shown in the with PHMB,
insert, the and optical photographs:
characteristic peak of (C) untreated
cellulose at 3330cotton
cm −1 fabric
becomesand stronger
(D) PHMB-coated
after coating
treated with PHMB, and optical photographs: (C) untreated cotton fabric and (D) PHMB-coated fabric
withfabric
PHMB,
dyed
dyed with demonstrates
withwhich
bromophenol blue
bromophenol blue (BPB).that(BPB).
PHMB was successfully coated on the cotton fabric.

3.2. FTIR Measuremnt

FTIR analysis was conducted to confirm the presence of PHMB on the treated cotton fabric, as
shown in Figure 3. A sharp and strong absorbance peak at 1550 cm−1 was observed in the spectrum
of PHMB, characteristic of imine group. The broad double peaks at 3195 cm−1 and 3380 cm−1 are
ascribed to stretching vibration of –NH- and –NH2- of PHMB molecule. Compared to PHMB, the
absorption spectrum of cellulose is pretty weak, particularly for the untreated control cotton fabric.
As shown in the insert, the characteristic peak of cellulose at 3330 cm−1 becomes stronger after coating
with PHMB, which demonstrates that PHMB was successfully coated on the cotton fabric.

Figure 3.
Figure 3. FTIR
FTIR absorbance
absorbance spectra
spectra of
of PHMB,
PHMB, untreated
untreated cotton
cotton fabric
fabric and
and PHMB-coated
PHMB-coated cotton
cotton fabric.
fabric.
The insert
The insert shows
shows the
the spectrum
spectrum of
of untreated
untreated cotton
cotton and
and treated
treatedcounterpart.
counterpart.

3.3. Effect of Concentration of PHMB on Antibacterial Activity

In order to explore effects of PHMB on the antibacterial activity, different concentrations were
further studied (Figure 4). It can be clearly seen that all the samples treated with different amounts of
PHMB show strong inhibition against S. aureus and K. pneumonia. Table 2 shows that the concentration
of PHMB had a significantly positive relationship with antibacterial activity. It is noteworthy that the
antibacterial activity for concentration of 2.5 and 5% was not significant. A significant antibacterial
ability was 3.
Figure seen forabsorbance
FTIR concentrations
spectraof
of10 and 15%,
PHMB, however.
untreated cotton fabric and PHMB-coated cotton fabric.
The insert shows the spectrum of untreated cotton and treated counterpart.
 In order to explore effects of PHMB on the antibacterial activity, different concentrations were
further studied (Figure 4). It can be clearly seen that all the samples treated with different amounts
of PHMB show strong inhibition against S. aureus and K. pneumonia. Table 2 shows that the
concentration of PHMB had a significantly positive relationship with antibacterial activity. It is
noteworthy
Coatings that
2020, 10, 520 the antibacterial activity for concentration of 2.5 and 5% was not significant. A
6 of 13
significant antibacterial ability was seen for concentrations of 10 and 15%, however.

Figure
Figure 4. Qualitative
4. Qualitative assayassay for
for the the antibacterial
antibacterial activityactivity of PHMB-coated
of PHMB-coated fabricsS.
fabrics against aureus S.
against andaureus and
K. pneumonia.
K. pneumonia.
Table 2. Effect of concentration of PHMB on antibacterial activity.
Table 2. Effect of concentration of PHMB on antibacterial activity.
Inhibition Zone/mm
Sample PHMB Conc./% Inhibition K.
zone/mm
Sample PHMB Conc./% S. aureus pneumoniae
S. aureus K. pneumoniae
Control 0 0 0
Control
1 0
2.5 4.50 0
3.5
21 2.5
5 4.5
4.5 3.5
5.5
32 105 4.5
4.75 5.5
6.75
43 10
15 4.75
6.75 6.75
7.25
4 15 6.75 7.25
3.4. Effect of Detergent on Antibacterial Activity
3.4. Effect of Detergent on Antibacterial Activity
In practical application, medical textiles are inevitably subjected to simulated healthcare laundering.
Frequentpractical
In laundering application,
generallymedical textiles
has a serious are inevitably
negative influencesubjected to simulated
on the antibacterial healthcare
activity of the
laundering.
treated fabric.Frequent
Therefore,laundering
durability generally
against has a serious
laundering negative
is of influence on
high importance for the antibacterial
medical textiles.
activity
This studyof is
the treated
thus focused fabric. Therefore,
on the durability laundering
effect of healthcare against laundering
washing is onof
thehigh importance
antibacterial for
ability.
medicalwe
Firstly, textiles.
studied Thisthestudy
effectisofthus focused on
commercial the effect
detergent on of healthcare activity
antibacterial laundering washing
against on the
S. aureus of
antibacterial
treated fabric ability.
samples. Firstly, we studied
The fabric sample theusedeffect ofexperiment
in this commercialwas detergent on antibacterial
not treated with PHMB, butactivity
was
against
just S. aureus
subjected of treated
to the washing fabric
test. samples. The fabric
Table 3 shows sample
the results ofused in this
samples experiment
washed was not
by detergent treated
with and
with PHMB,
without but was
bleaching justsodium
agent subjected to the washing
hypochlorite (300test. Table
ppm). 3 shows
It was found the results
that of samples
addition washed
of commercial
by detergent
detergent with
in the and without
washing solution bleaching agentinhibition
shows strong sodium hypochlorite (300against
and disinfection ppm). It
S. was found
aureus, and that
this
addition of commercial detergent in the washing solution shows strong inhibition
effect is irrespective of the number of washing cycles. Moreover, the fabric samples showed yellowing and disinfection
against
after S. aureus,
being washed andwiththisthe
effect is irrespective
addition of the number
of the bleaching of washing
agent sodium cycles. Moreover, the fabric
hypochlorite.
samples showed yellowing after being washed with the addition of the bleaching agent sodium
hypochlorite. Table 3. Antibacterial properties of untreated samples washed by detergent.

Detergent Detergent + NaClO

Washing Cycles
Inhibition/% 1 Disinfection/% 2 Inhibition/% 1 Disinfection/% 2
Control, no wash 0 0 0 0
26 0 100 0 100
52 0 100 0 100
104 0 100 0 100
1 Inhibitory % = [(control after 18 h) – (specimen after 18 h)]/[control after 18 h] × 100%. 2 Disinfectant % = [(control
after 0 h] – [specimen after 18 h)]/[control after 0 h] × 100%.

3.5. Effect of Washing Cycles on Antibacterial Activity

Table 4 shows the effects of washing cycles on the antibacterial activity against S. aureus and
K. pneumonia of PHMB coated fabric samples. As shown in Table 4, after 52 washing cycles, the fabric
 52 0 100 0 100
104 0 100 0 100
1 Inhibitory % = [(control after 18 h) – (specimen after 18 h)]/[control after 18 h] × 100%. 2 Disinfectant % =
[(control after 0 h] – [specimen after 18 h)]/[control after 0 h] × 100%.
Coatings 2020, 10, 520 7 of 13
3.5. Effect of Washing Cycles on Antibacterial Activity
Table 4 shows the effects of washing cycles on the antibacterial activity against S. aureus and K.
samples still showed strong inhibition and disinfection, against both S. aureus and K. pneumonia.
pneumonia of PHMB coated fabric samples. As shown in Table 4, after 52 washing cycles, the fabric
However, a clear decrease was observed in the antibacterial ability for the samples after 104 washing
samples still showed strong inhibition and disinfection, against both S. aureus and K. pneumonia.
cycles. This indicates that simulated healthcare laundering has a significant influence on antibacterial
However, a clear decrease was observed in the antibacterial ability for the samples after 104 washing
activity of treated fabrics, and the coated samples show excellent durability against washing.
cycles. This indicates that simulated healthcare laundering has a significant influence on antibacterial
activity of treated fabrics, and the coated samples show excellent durability against washing.
Table 4. Antibacterial properties of treated samples washed by different cycles.
The qualitative analysis of PHMB-coated fabric samples was also conducted via dyeing with
BPB. As seen in Figure 5, it clearly shows that the1 blue complex salt Disinfection/%
Inhibition/% was significantly
2
formed on the
Washing Cycles
treated samples, which demonstrates
S. aureusthat PHMB still
K. pneumoniae existed on the
S. aureusfabric samples after different
K. pneumoniae
washing cycles.no wash 100 100 100 100
26 100 100 100 100
Table
52 4. Antibacterial100 properties of treated
100 samples washed 100 by different cycles.
100
104 95 38.6 0 0
Inhibition/% 1 Disinfection/% 2
Washing
1 InhibitoryCycles
% = [(control after 18 h) − (specimen after 18 h)]/[control after 18 h] × 100%. Disinfectant % = [(control
2
S. aureus K. pneumoniae S. aureus K. pneumoniae
after 0 h] − [specimen after 18 h)]/[control after 0 h] × 100%.
no wash 100 100 100 100
26 100 100
The qualitative analysis of PHMB-coated fabric samples was also conducted via dyeing 100 100 with
52 100 100 100
BPB. As seen in Figure 5, it clearly shows that the blue complex salt was significantly formed 100 on the
104 95 38.6 0 0
treated samples, which demonstrates that PHMB still existed on the fabric samples after different
1 Inhibitory % = [(control after 18 h) − (specimen after 18 h)]/[control after 18 h] × 100%. 2 Disinfectant % =
washing cycles.
[(control after 0 h] − [specimen after 18 h)]/[control after 0 h] × 100%.

Figure 5.
Figure 5. Qualitative
Qualitative test
test results
results of
of PHMB-coated fabric samples
PHMB-coated fabric samples dyed
dyed with
with BPB:
BPB: (A)
(A) pristine
pristine uncoated
uncoated
fabric; (B)
fabric; (B) no
no wash;
wash; (C)
(C) 26
26 washing
washing cycles;
cycles; (D)
(D) 52
52 washing
washing cycles;
cycles; and
and (E)
(E) 104
104 washing
washingcycles.
cycles.

3.6. Tearing
3.6. Tearing Strength
Strength Analysis
Analysis
Figure 66presents
Figure presentsthat
thatthe
the effects
effects of scouring,
of scouring, coating
coating and and washing
washing on tearing
on tearing strength
strength of the of the
fabric
fabric substrate.
substrate. Clearly,Clearly, for the sample,
for the control control tearing
sample,strength
tearing instrength in both
both warp and warp and weft was
weft directions directions
found
was
to befound to be the
the highest highest to
compared compared
the othertosamples.
the otherThere
samples. There
is an is anreduction
obvious obvious reduction
in tearinginstrength
tearing
strength
of of fabricafter
fabric samples samples after indicating
scouring, scouring, indicating thathas
that scouring scouring has aeffect
a negative negative effect strength
on tearing on tearing
of
strength of fabrics. Likewise, after coating the scoured fabrics, tearing strength in the warp direction
fabrics. Likewise, after coating the scoured fabrics, tearing strength in the warp direction dropped
from 28.44 to 24.07, whereas the weft direction saw a decrease from 28.89 to 24.45. Then, the coated
fabric sample was washed 104 times and tearing strength sharply declined to 14.7 and 13.86, for warp
and weft direction, respectively. The results demonstrate that scouring, coating and washing treatment
have a significant negative influence on tearing strength, particularly washing.
Figure 7 shows that the effect of washing conditions on tearing strength. It can be clearly seen that
there was no significant difference between washing temperature 65 ◦ C and 75 ◦ C. Compared with
simulated healthcare washing, tearing strength of treated fabrics has an obvious decrease, but it is
still higher than that of washed samples. This demonstrates that the strength loss for treated samples
is acceptable.
 Coatings 2020, 10, x FOR PEER REVIEW 8 of 13

dropped from 28.44 to 24.07, whereas the weft direction saw a decrease from 28.89 to 24.45. Then, the
coated fabric sample was washed 104 times and tearing strength sharply declined to 14.7 and 13.86,
for warp
Coatings 2020,and weft direction, respectively. The results demonstrate that scouring, coating and washing
10, 520 8 of 13
treatment have a significant negative influence on tearing strength, particularly washing.

Figure 6. Tearing strength of control sample, scoured, coated, and washed samples (104 washing
cycles, 65 oC with nonionic detergent but without bleaching agent); warp (A) and weft (B).

Figure 7 shows that the effect of washing conditions on tearing strength. It can be clearly seen
that there was no significant difference between washing temperature 65 °C and 75 °C. Compared
with simulated healthcare washing, tearing strength of treated fabrics has an obvious decrease, but
it is still
Figure higher
Figure 6. 6. thanstrength
Tearing
Tearing that ofofwashed
strength samples.
of control
control sample,
sample, This demonstrates
scoured,
scoured, coated,
coated, and that the samples
washed
and washed strength
samples loss
(104 for treated
washing
(104 washing cycles,
samples is acceptable.
◦ C with nonionic
65cycles, 65 oC with nonionic detergent
detergent but without
but without bleaching
bleaching agent); agent);
warp (A)warp
and(A) and(B).
weft weft (B).

Figure 7 shows that the effect of washing conditions on tearing strength. It can be clearly seen
that there was no significant difference between washing temperature 65 °C and 75 °C. Compared
with simulated healthcare washing, tearing strength of treated fabrics has an obvious decrease, but
it is still higher than that of washed samples. This demonstrates that the strength loss for treated
samples is acceptable.

Figure
Figure 7.
7. Tearing strengthofofcontrol
Tearing strength control and
and treated
treated samples
samples afterafter 52 washing
52 washing cycles
cycles at 65 at
◦ C65 °C75and
and ◦ C,75 °C,
warp.
warp.
3.7. Hand Feel Measurement
3.7. Hand Feel
In the Measurement
project, antibacterial finishing formulation was fully investigated to assess its effect on the
handInfeel
theproperty,
project, antibacterial
as shown in finishing
Table 5. formulation was fully investigated to assess its effect on the
hand feel property,
Figure as strength
7. Tearing shown in of Table
control5.and treated samples after 52 washing cycles at 65 °C and 75 °C,
warp. Table 5. The different antibacterial recipes for fabric samples antibacterial treatment.

Sample PHMB (%, v/v) PEG (%, v/v) Binder (%, v/v)
3.7. Hand Feel Measurement
G1 5 5 5
In the project, antibacterial
G2 finishing
5 formulation was
3 fully investigated5to assess its effect on the
hand feel property, as
G3shown in Table 5. 5 1 5
G4 5 0 5
G5 5 5 3
G6 5 3 3
G7 5 1 3
G8 5 0 3

After coating with above recipes, the samples were then assessed in terms of hand feel properties,
such as resilience, softness, and smoothness, etc., as shown in Table 6. Clearly, compared to the control
sample, hand feel properties show a significant decrease in terms of resilience, softness, and smoothness.
This indicates that the antibacterial treatment has a negative impact on the hand feel of fabrics. Likewise,
Coatings 2020, 10, 520 9 of 13

an obvious decline in whiteness was also observed after coating with PHMB recipe. This demonstrates
that antibacterial treatment has a slightly negative influence on the performance of fabrics.

Table 6. Hand feel properties of fabric samples coated with different antibacterial recipes.

Sample Resilience Softness Smoothness HFI Whiteness

Control 82.3 78.4 82.3 243.0 84.6
G1 80.3 76.7 81.2 238.2 83.9
G2 82.4 77.3 81.2 240.9 83.5
G3 83.0 77.4 81.5 241.9 82.4
G4 82.9 78.1 81.3 242.3 84.2
G5 82.2 78.6 81.6 242.4 83.2
G6 82.3 78.4 81.2 241.9 84.2
G7 83.0 77.2 81.8 242.0 82.5
G8 82.9 77.4 81.9 242.2 83.2

Next, the effect of washing on performance of textile fabrics was further investigated (Table 7).
Compared to Table 6, HFI values of all the samples significantly decreased after washing, which indicates
that washing has an obvious influence on the hand feel of textiles. Meanwhile, the whiteness also saw
a sharp decrease from 80+ to 60+, particularly for the coated samples. This may be due to the loss
of fluorescent whitening agent after washing because they are often used for textiles to improve the
whiteness [29,30].

Table 7. The hand feel properties of PHMB coated fabric samples after washing (104 cycles, 65 ◦ C).

Sample Resilience Softness Smoothness HFI Whiteness

Control 79.3 78.0 79.5 236.8 82.7
G1 80.2 76.4 80.1 236.7 61.1
G2 79.8 76.4 79.7 235.9 63.5
G3 80.5 76.4 80.4 237.3 63. 2
G4 80.3 76.6 78.0 234.9 61.9
G5 80.8 76.8 80.6 238.2 62.3
G6 79.6 77.2 79.2 236.0 61.0
G7 80.0 76.7 80.0 236.7 63.6
G8 81.3 76.9 80.4 238.6 61.9

4. Discussion
PHMB is a cationic biocide marketed worldwide due to its excellent antibacterial activity, chemical
stability, low toxicity, and reasonable cost, and has been extensively utilized in textile industry [3,7].
However, a common issue facing PHMB-coated fabrics is the durability against household laundering.
The present study explored the effects of various parameters, such as washing cycles and household
detergents, on the antibacterial activity of PHMB-coated fabric samples, as well as effects of PHMB
formulation on the physical properties of cotton substrate, including tearing strength and hand
feel value.
From SEM observation, the presence of PHMB was confirmed, and the stable blue complex was
formed with BPB dyebath (Figure 2). The characteristic absorption peak of cellulose was also enhanced
due to the coating of PHMB (Figure 3). The PHMB-coated fabric samples exhibit prominent inhibition
activity against S. aureus and K. pneumonia (Figure 4). Moreover, the antibacterial behavior of PHMB
was shown to a concentration dependent effect. However, there is no significant difference between
the concentrations of 2.5% and 5% PHMB in the antibacterial behavior, while, for 10% and 15% PHMB,
a significant antibacterial activity was observed (Table 3). The effectiveness against cellular organisms
is due to the positively charged biguanide group attached to a flexible spacer. PHMB binds to the
negatively charged phosphate head groups of phospholipids at bacteria cell wall or virus envelope,
Coatings 2020, 10, 520 10 of 13

causing increased rigidity, sinking non-polar segments into hydrophobic domains, disrupting the
membrane with subsequent cytoplasmic shedding, and culminating in cell death [16].
Durability against household laundering is an important property for medical textiles. Originally,
we performed the washing tests with the commercial household detergent added to simulate the
practical application scenario. However, it was found that the antibacterial properties of washed
samples were seriously interfered by the commercial detergent, the possible reason of which may be
the addition of some additives with microbicidal efficacy (Table 3). Therefore, a non-ionic surfactant
7EO was used for further experiments. The bleaching agent sodium hypochloride was abandoned due
to the fabrics yellowing caused.
Next, we performed the antibacterial experiments on treated fabrics against two bacteria: S. aureus
and K. pneumonia to pinpoint the effect of simulated healthcare laundering on the antibacterial ability.
The fabric samples were shown strong bactericidal effect against both bacteria after 52 washing cycles
(Table 4). The attenuated bactericidal activity was still observed in the samples with 104 washing
cycles, which was further confirmed by BPB dyeing tests (Figure 5). This shows that frequent washing
may negatively influence the antibacterial ability of PHMB-coated fabrics. In spite of this, the washing
experiments demonstrate that the fabric samples treated with PHMB formulation possess satisfactory
durability against washing. Similar results were also reported by Chen and coworkers [31]. In their
study, PHMB was padded on the fabric and then dried at 120 ◦ C for 5 min. PHMB-coated fabric
samples still showed excellent antimicrobial property against S. aureus (99%) and K. pneumonia (94%)
after 25 washing cycles. Gao et al. coated PHMB on the wool fabric by exhaustion method and studied
the antibacterial behaviors against gram-negative bacteria E. coli [32]. They found that PHMB-coated
wool fabric was durable to 5 accelerated washing cycles (ISO 5A cycle, equivalent to 40–50 wool
washing cycles) and maintained 99% bacterial reduction for 8% PHMB treated samples. In the present
study, the durability against laundering was dramatically increased to almost 104 washing cycles by
optimizing the finish process. On the one hand, the underlying reason may be the electrostatic attraction
between PHMB and cellulosic molecules [33], which is enhanced by the addition of polyurethane
binder and high-temperature curing. On the other hand, polyurethane binder acts as a cross-linker and
form hydrogen bond with PHMB and cellulosic molecules, which eventually enhance the durability
property of PHMB treated fabrics [34].
Tearing strength of fabric is affected by many parameters, such as fiber structure and post-finishing
process. The present study investigates the effects of scouring, coating, and washing on tearing
strength of the fabric (Figure 6). Compared to the control sample, tearing strength of the fabrics were
clearly debased after treatment, particularly after washing. In this study, the samples were firstly
subjected to scouring treatment to remove the impurities, which slightly decrease the tearing strength
of fabrics. And then, the scoured samples were coated with PHMB formulation via pad-dry-cure
process, which further deteriorate the tearing strength. Accordingly, the tearing strength of the coated
fabrics were gravely undermined after 104 washing cycles, the potential reason of which may be
the hydrolysis of cellulosic fibers [35,36]. However, the effect of washing temperature on the tearing
strength was not significant, even though a much strength loss was observed with a higher washing
temperature (75 ◦ C) (Figure 7).
Finishing treatment and regular washing generally have an obvious negative influence on the
hand feel of a fabric [37,38], as confirmed in Tables 6 and 7. For the samples of G1–G4, which were
coated with different concentrations of PEG, there is an increase in the value of HFI, indicating that the
reduction of PEG helps enhance the hand feel performance of fabrics. Looking at samples of G5–G8,
concentration of the binder dropped from 5% to 3% and effects of PEG on the hand feel was further
investigated. It can be found that HFI values increased, excluding the sample G5. Overall, HFI values
of samples G5–G8 were higher than G1–G4 samples, which was due to the smaller amount of PHMB
formulation used for the coating (Table 6). By contrast, HFI values of all the samples significantly
decreased after washing, which indicates that washing has an obvious influence on the hand feel of
textiles, and the whiteness also sharply decreased (Table 7).
Coatings 2020, 10, 520 11 of 13

In summary, the fabric samples coated with PHMB formulation show excellent antibacterial
activity against S. aureus and K. pneumonia. Washing test shows that washing has a significantly
negative influence on the antibacterial activity, tensile strength and hand values. However, the samples
prepared by the optimum process exhibit satisfactory durability for simulated healthcare laundering.

5. Conclusions
Durability against simulated healthcare washing is an important property for medical textiles.
The durability property can be achieved by optimizing the finishing process. It was found that the
optimum finishing conditions can impart excellent durability to fabrics expected to undergo repeated
simulated healthcare washing. After 104 washing cycles, the PHMB-coated fabric samples still show
distinct inhibition activity, particularly against S. aureus. Additionally, the present study also shows
that both simulated healthcare washing and coating treatment have negative influence on the hand
feel behavior and tearing strength of cotton fabric. Therefore, the antibacterial finishing for textiles
should not neglect the negative influence on the materials.

Author Contributions: Conceptualization, J.C., J.Y., K.-F.Y., and C.-W.K.; Data curation, W.-Y.W.; Formal analysis,
W.-Y.W., J.-C.C., and C.-W.K.; Funding acquisition, C.-W.K.; Investigation, W.-Y.W.; Methodology, W.-Y.W., J.-C.C.,
and C.-W.K.; Project administration, C.-W.K.; Supervision, C.-W.K.; Validation, W.-Y.W.; Visualization, W.-Y.W.;
Writing-original draft, W.-Y.W.; Writing-review & editing, C.-W.K. All authors have read and agreed to the
published version of the manuscript.
Funding: This research was funded by The Hong Kong Polytechnic University, grant numbers ZVNM and ZVQJ.
Acknowledgments: The authors would like to thank the financial support from The Hong Kong Polytechnic
University for this work under the project of account codes: ZVNM and ZVQJ.
Conflicts of Interest: The authors declare no conflict of interest.

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