Journal of Cleaner Production 336 (2022) 130465

Contents lists available at ScienceDirect

Journal of Cleaner Production

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

Sonochemical mordanting as a green and effective approach in enhancing

cotton bio natural dye affinity through soy surface modification
Yanyun Zhang , Qi Zhou , Weibang Xia , Luqman Jameel Rather , Qing Li *
State Key Laboratory of Silkworm Genome Biology, Chongqing Engineering Research Center for Biomaterial Fiber and Modern Textile, College of Sericulture, Textile and
Biomass Science, Southwest University, Chongqing, 400715, China

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

Handling Editor: Prof. Jiri Jaromir Klemeš As a clean technology, ultrasonics has been widely explored in textile dyeing. Mordanting is commonly used for
the achievement of efficient textile dyeing, however little attention has been paid on application of ultrasonics in
Keywords: mordanting. This study investigated sonochemical mordanting and its efficiency in subsequent dyeing. Ultrasonic
Cotton bath, together with traditional water bath and magnetic stirring bath were investigated. Soy protein and
Ultrasonics
F. Artemisiae argyi (FAA) were used as a mordant and natural dye, due to the their natural compatibility with
Mordanting
cotton as well as biological properties. All the materials used in this work were natural with very little chemicals
Soy protein
Bio natural dye (present no harm to the environment) applied. Results showed that while soy mordanting in water bath can
Antibacterial significantly increase fiber natural dye uptake, the dye affinity can be enhanced further when ultrasonic irra­
diation was applied. Ultrasonic mordanting was found to be able to produce higher fabric color strength (K/S)
while consuming less soy protein when compared with other mordanting baths. Less weight increase as a result
of ultrasonic irradiation can also provide cotton fabric with softer handle than those processed in traditional
water bath. UV protection of dyed fabrics was found to be significantly improved from the control sample, with
samples processed with ultrasonics showing the greatest improvement. In addition to the increased dye affinity
as a result of soy mordanting, fabric bio function of antibacterial property was found to be simultaneously and
successfully achieved.

1. Introduction
As the most commonly used natural fiber, cotton remains the biggest
global natural fiber production and clothing consumption to date (Wang
and Memon, 2020). Cotton is the most important cellulose fiber with
natural characteristics such as comfort, softness, bio degradable, and
excellent hygroscopicity/air permeability.
Application of natural dye in textile dyeing has gained massive
attention and popularity in recent years due to environmental and
health concern. Textile dyed with natural dye, however, is generally
poor in color fastness (especially light fastness) which limited the wide
usage of natural dye. Metal ion mordants are traditionally applied in
dyeing process to increase fiber natural dye affinity by forming
complexation and hence color fastness of dyed textile can be improved.
However the use of metal salt mordants can result in discharging metal
ions in waste water, therefore is considered as environmental un­
friendly. Research into replacement of traditional metal ion mordants
with natural bio mordants has become popular in recent years (Adeel
et al., 2021; Habib et al., 2021; Zhang et al., 2021), owing to green
nature of the materials as well as their effectiveness in the improvement
of textile dyeing with natural dye.
Plants extracts, such as carotenoids, xanthophylls, flavonoids, and
anthocyanin, are common source for natural dye. Unlike protein fibers
of wool and silk which can form complexation with natural dye (Rat­
tanaphani et al., 2007), cotton carries a small negative charges due to
the presence of hydroxyl groups (Fig. 1a). The negative charges on the
surface of cellulose fibers present repulsion to phenolic hydroxyl groups
(which also carry negative charges) commonly found in natural dyes.
Therefore natural dye affinity of cotton is generally poor. Studies have
been conducted to overcome the problem, much of which are focused on
cationic surface modification using synthetic agents (Eorn et al., 2001;
Janhom et al., 2004; Ben Ticha et al., 2013; Rym et al., 2016) or
chemical compounds containing amine, such as chitosan and protein
(Rattanaphani et al., 2007; Pisitsak et al., 2016; Pisitsak et al., 2017;
Saleh et al., 2019; Haji, 2020).
Ultrasonics is a green technology. Ultrasonic assisted textile wet

* Corresponding author.
E-mail address: qingli@swu.edu.cn (Q. Li).

https://doi.org/10.1016/j.jclepro.2022.130465
Received 22 August 2021; Received in revised form 7 January 2022; Accepted 8 January 2022
Available online 10 January 2022
0959-6526/© 2022 Elsevier Ltd. All rights reserved.
Y. Zhang et al.
processing has been widely studied, with some reported on natural
dyeing of cotton (Kamel et al., 2009; Vankar et al., 2007; Adeel et al.,
2019; Baig et al., 2020). Much of the studies are, however, conducted in
dyeing process. Applying ultrasonics in the mordanting stage seems to
have received very little attention. This work examines the use of ul­
trasonic irradiation during mordanting. Ultrasonics bath is compared
with traditional water bath and magnetic stirring bath in the mordanting
process.
Soy and F. Artemisiae argyi (FAA) are used as mordant and natural
dye in this work. Soybean is abundant in nature and is inexpensive.
Various amino acids are found in soy protein, with lysine and methio­
nine being the two essential amino acids (McAdams, 2021) (Fig. 1b).
FAA is widely distributed in nature, and is known as traditional herbal
medicine used in healthcare in China. Eupatilin and jaceosid (Fig. 1c)
are the two major bio colorants/dyes, with natural green-yellowish color
that can be extracted from FAA (Rather et al., 2020).
Same as cotton, both soy and FAA are natural crop/plant products
with non-animal origin and are safe to use. A simple water bath
extraction (50% ethanol) is used to produce natural dye in this work.
Very little amount of chemicals used for adjusting pH of dye bath are
acetic acid and sodium bicarbonate, which can be used in food pro­
duction therefore present no harm to the environment. Ultrasonics is
known as a clean technology. This study is expected to provide a green
and clean cotton natural dyeing production with a significantly
enhanced color strength and bio function seen in the final products.
2. Experimental
2.1. Materials and chemicals
Undyed, 100% pure cotton plain woven fabric with areal weight of
105 g/m2 (purchased from local textile mill) was used in this study. Soy
protein powder was of food grade, purchased from Henan Zhongtai Food
Chemical Co., Ltd, China. Leaves of F. Artemisiae argyi (FAA) were
sourced from local market, and were cleaned, dried and ground into fine
powder using a electric grinder before dye extraction. Dye extraction
was conducted using a simple water bath (50% ethanol) extraction
method described in a previous study (Rather et al., 2020).
Ethanol (99%), acetic acid (CH3COOH), sodium bicarbonate
(NaHCO3), and chemicals used in antibacterial test, such as sodium
chloride (NaCl) and potassium persulphate (K2S2O8) were of laboratory
grade.
2.2. Fabric mordanting and dyeing process
Three mordanting baths were investigated in this work. Traditional
Fig. 1. Chemical structures of a) cellulose, b) lysine and methionline from soy protein, and c) natural colorant of eupatilin and jaceosidin from F. Artemisiae
argyi (FAA).
2
Journal of Cleaner Production 336 (2022) 130465
water bath was conducted in a SHZ-C constant temperature water bath
(Changzhou Nuoji Instrument Co., Ltd., China). Ultrasonic bath used
was a 40 kHz ultrasonic water tank with temperature control (HS Ul­
trasonic Solution Co., Ltd., China). Magnetic stirring bath was conducted
in a DF-101S heat-collecting constant temperature heating magnetic
agitator (Gongyi Yuhua Instrument Co., Ltd, China).
Cotton fabric samples were immersed in the various mordanting
baths with soy concentrations of 1–6% at temperature of 60 ◦ C for 60
min. Fabrics were then taken out and padded twice through a little
padding mangle before drying at room temperature. Fabric dyeing was
conducted in extracted FAA dye solution with a liquor to fabric ratio of
50:1. pH of dye bath was set at soy protein iso-electric point of pH 5 (Lee
et al., 2021). Temperature of dye bath was raised from ambient to 85 ◦ C
at a heating rate of 2 ◦ C per min, and then maintained at 85 ◦ C for 90
min. After dyeing, fabric samples were taken out and thoroughly rinsed
with deionized water before drying in shade at room temperature.
2.3. Evaluation for fiber surface morphology
A Phenom ProX SEM (Nanoscience, Pheoenix AZ, USA) equipped
with Energy Disperse X-ray Spectroscopy (EDS) instrumentation for
elemental composition analysis, was used to record fiber surface
morphology, under an Extra High Tension of 10 kV.
2.4. Evaluation for weight increase, bending rigidity, and fabric tensile
properties
Percentage fabric weight increase was evaluated by calculating
fabric weight change before and after mordant dyeing, relative to the
fabric weight before mordant dyeing, using Equation (1). Fabric samples
were conditioned at 20 ± 2 ◦ C and 65 ± 2% relative humidity for 24 h
before weighing.
Weight increase (%) ​ =
Wa − Wb
× 100% (1)
Wb
where Wb refers to fabric weight before mordant dyeing, and Wa fabric
weight after mordant dyeing.
Fabric bending length was measured by a YG022D automatic fabric
stiffness tester (Wenzhou Darong Textile Instrument Co. Ltd., China).
Fabric bending rigidity (stiffness) was calculated using Equation (2),
according to GB/T18318.1.
G = m × (L/2)3 × 10− 3
(2)
Where G refers to fabric bending rigidity per areal weight (mN⋅cm), m
fabric areal weight (g/m2), and L bending length of the fabric sample
(cm).
Y. Zhang et al. Journal of Cleaner Production 336 (2022) 130465

Tensile testing was conducted using an Exceed Model E44 tensile

machine (MTS Systems Co. Ltd., China) with a gauge length of 136 mm
at an extension rate of 2 mm/min. Samples with 10 mm in width were
cut from each fabric. Experiments were carried out in standard condition
of 20 ± 2 ◦ C and 65 ± 2% relative humidity. At least 4 measurements
(both warp and weft) were conducted and results were averaged. Fabric
percentage strength loss (%) and extension gain (%) were calculated
using Equations (3) and (4).
Lc − Ld
Strength loss ​ (%) ​ = × 100% (3)
Lc

Ed − Ec
Extension gain ​ (%) ​ = × 100% (4)
Ec

where Ld and Ed refer to maximum load at break (N/mm2) and extension

at break (mm) for dyed fabric, and Lc and Ec maximum load at break (N/
mm2) and extension at break (mm) for fabric without mordant dyeing
(used as control).

2.5. Measurement of color strength K/S and color fastness

Color strength (K/S) of dyed cotton fabrics was obtained from a

650TM Spectrophotometer (Datacolor, USA). Each fabric piece was
measured 10 times and results were averaged.
Wash fastness and rubbing fastness were evaluated following the
standard testing methods of ISO 105-C06:1994 and ISO 105/X12:2001,
using a DigiWASH-SS (Yuanmao Co. Ltd., China) and a Digi Crockmeter
(Changken Testing Equipment Co. Ltd., China). Light fastness was tested
according to the standard of AATCCTM16-2003 using an Xenon lamp
accelerated aging test box (Changken Testing Equipment Co. Ltd.,
China).

2.6. Evaluation for UV protection and antibacterial properties

UV index was measured by an YG912E textile UV resistance tester
(MEBON Ltd., China), according to EU standard 13758-2001. At least 5
measurements were conducted for each sample and results were aver­
aged. Antibacterial activity of dyed cotton fabrics was assessed using an
absorption method in accordance with testing standard of GB/T
20944.2-2007. Staphylococcus aureus (MTCC902, Gram-positive) and
Escherichia coli (MTCC443, Gram-negative) were used as experimental
strains.
3. Results and discussions
3.1. Effects of soy protein mordanting on natural dyeing of cotton
Soy protein mordanting of cotton was investigated in various mor­
danting baths, and results of color strength of dyed fabrics are shown in
Fig. 2. It is seen from Fig. 2a that when fabric dyed without mordant (0%
soy concentration), K/S < 2 was observed in all cases. Upon mordanting,
K/S of dyed fabric increased significantly in all the mordanting baths
investigated. A progressive raise of color strength K/S is seen as soy
concentration increased from 1% to 6%, indicating that soy concentra­
tion in mordanting process played an important role in attracting nat­
ural dye. Images of fabric shade in Fig. 2b echo the results shown in
Fig. 2a. It can be seen that natural green-yellowish colorant from FAA
are evenly and increasingly adsorbed by the fabric as soy concentration
increases.
The observed soy mordant induced increase in fabric color strength
can be varied when mardanting is processed in different baths. It is seen
in Fig. 2a that ultrasonic mordanting bath exhibited the best perfor­
mance in attracting natural dye, followed by water bath and magnetic
stirring bath. This is expected and can be related to the mechanism of
ultrasonic assisted wet processing, during which time energy generated
from the cavitation bubble implosion is responsible for a quick and
Fig. 2. (a–b). Color strength of dyed cotton fabrics vs soy concentration in
various mordanting baths, (a) K/S value of dyed fabrics; (b) Images of dyed
fabrics at various soy concentrations. (For interpretation of the references to
color in this figure legend, the reader is referred to the Web version of
this article.)
efficient fiber mordant uptake (Pan et al., 2018). Magnetic stirring is the
lest effective approach among the three baths investigated. This is
because unlike still water bath, magnetic stirring can generate turbulent
flow in the bath and can be disturbing for soy molecules to settle on the
fibre surface.
Fig. 3 presents the chemical interaction of cotton cellulose - soy
protein - natural dye of Eupatilin extracted from FAA. It is seen that bio
mordant of soy protein is able to firstly form soy-cellulose complex
during mordanting process (which can be accelerated by applying ul­
trasonic irradiation), and then followed by soy-dye connection in
dyeing. Soy protein as a mordanting agent acted effectively as a bridge
between the cellulose fiber and natural dye. Soy mordant at a higher
concentration produces a greater number of protein molecules, which
can result in a higher rate of fabric dye uptake reflected by K/S value
measured in Fig. 2a.
Following these analysis, it is believed and expected that ultrasonic
assisted soy protein mordanting of cotton applied in this work (Fig. 4) is
capable of providing cotton fabric with enhanced natural coloration and
bio functional finish.
3.2. Effects of ultrasonic mordanting on dyeing efficiency
3.2.1. Changes in fiber surface morphology
Fig. 5 of SEM images unveiled changes of fiber surface morphology
before and after mordanting. While little difference is seen from fiber
cross section, it is clearly shown in longitudinal images that compared
with fibers with smooth surface before treatment (Fig. 5a), soy coating is

3
Y. Zhang et al. Journal of Cleaner Production 336 (2022) 130465

Fig. 3. Ultrasonics assisted chemical interaction of cotton cellulose-soy mordant-natural dye.

Fig. 4. A schematic diagram of eco-friendly process of cotton for the enhancement of natural coloration and bio functional finish.

Fig. 5. (a–c). SEM images of longitudinal and cross-sectional cotton fibers before and after soy mordanting (at soy concentration of 3%), a) before mordanting, b)
mordanted in water bath, and c) mordanted in ultrasonic bath.

4
Y. Zhang et al.
clearly produced on the fiber surface upon mordanting, in both water
bath (Fig. 5b) and ultrasonic bath (Fig. 5c). Difference between water
bath and ultrasonic bath lies in roughness of coating on the fiber surface.
It is seen that cotton fibers mordanted in water bath have a rougher
coating surface than that of ultrasonics. The roughness is presented in
the forms of uneven layers as well as fillings between gaps of the fibers,
as pointed by the yellow arrows in Fig. 5b. Ultrasonic bath, while pro­
duced the highest color strength of K/S values (Fig. 2a), is showing a
smoother fiber surface with less gap filling than that of the water bath.
These interesting observations could be due to the previously
mentioned cavitation implosion effect in the ultrasonic mordanting
process. At moments when ultrasonic irradiation induced cavitation
bubble imploded, it is able to generate a high velocity jet of water to pass
through centre of the bubble and strike the surface next to the bubbles
(Suslick, 1989). When soy particle next to the cavitation bubble is struck
by the high velocity fluid jet it is able to disintegrate agglomerated
particles, causing milling and mixing of soy cells, hence an easy diffusion
into the fibers.
EDS analysis (Fig. 6) from dyed cotton samples confirmed the
mordant dyeing effects. Very little change is seen (Fig. 6a and b) with
percentage carbon (C) composition before and after mordant dyeing,
whereas oxygen (O) is decreased and nitrogen (N) increased, both by 2%
after mordant dyeing. This observation suggested amino from soy pro­
tein present on the fiber surface. Combined with chemical interaction in
Fig. 3, it is clear that soy protein served as mordant acted effectively
between the cellulose fiber and nature dye.
Fig. 6. (a–b). Surface morphology and EDS analysis of cotton samples, a) before mordant dyeing and b) after mordant dyeing.
5
Journal of Cleaner Production 336 (2022) 130465
3.2.2. Dyeing efficiency, fabric handle and changes in fabric tensile
properties
As shown in SEM and EDS analysis, higher soy concentration in the
mordanting process might result in heavier coating on the fiber surface.
Although a subsequent improvement in dye uptake can be achieved
from the increasing soy coating (Fig. 2a), fabric handle might be
affected. The concern was investigated by measuring percentage weight
increase and bending rigidity of dyed fabrics, results of which are shown
in Fig. 7. In general, fabrics mordanted with higher soy concentration
have higher weight increase, and hence higher level of bending rigidity.
A higher level of fabric bending rigidity is responsible for an increased
stiffness of fabric handle. It is seen from Fig. 7a that water bath remains a
mordanting bath in gaining the highest weight and as a result, fabrics
show the highest bending rigidity (stiffness). Ultrasonic bath showed the
lest percentage weight increase with bending rigidity values much lower
than that of the water bath and similar to that of magnetic stirring bath
(Fig. 7b).
It can be seen from Figs. 7a and 2a, that fabric treated in ultrasonic
bath has gained the lest weight among the three mordanting baths
investigated whilst achieved the highest K/S values at various soy con­
centration applied. In other words, ultrasonic bath has enabled fabric to
achieve higher color strength (K/S) with less amount of soy protein
needed (less weight increase), when compared with that of water bath.
As agglomerated soy particles disintegrated in ultrasonic bath and
diffused into fibers with ease, less soy coating is attached to the surface
of fibers, therefore fabric handle is significantly improved. With mag­
netic stirring bath, although fabric handle is similar to that of ultra­
sonics, neither percentage weight increase (Fig. 7a) nor color strength
(Fig. 2a) are ideal. These results indicate that ultrasonic bath is the most
Y. Zhang et al. Journal of Cleaner Production 336 (2022) 130465

Fig. 7. (a–b). Weight increase (a) and binding rigidity (b) of dyed fabric vs soy concentration in different mordanting baths.

effective and efficient mordanting bath among the three baths investi­
Table 2
gated, and by using ultrasonic irradiation, fabric handle (softness) can
Color fastness of dyed cotton fabrics.
be greatly improved from that of traditional water bath.
In practice, a balance between dye affinity and fabric handle is sample color fastness

important in selecting soy concentration. Therefore dyed fabric with soy mordanting bath soy concentration wash rub light
mordant concentration of 3% was investigated further for fabric tensile type (%) fastness fastness fastness
properties, and results are shown in Table 1. dry wet
It is seen from Table 1 that regardless of bath type, there is a slight water bath 2 3–4 4–5 4 6
fabric strength loss (around 4–6%) from soy mordant dyeing. This could 3 3–4 5 4–5 6
be due to the fact that fabric dyeing was conducted in weak acidic 4 4 4–5 4 6
condition of pH 5, which could result in slight loss of fiber strength (Xu ultrasonic bath 2 3–4 4–5 4–5 5–6
3 4 4–5 4–5 6
and Li, 2000). The strength loss however, is at an acceptable level. Water
4 4 4–5 4 6–7
bath has seen an 6% loss of maximum extension. This could be explained magnetic stirring 2 3 4 4–5 6
from the results shown in Fig. 7 where water bath produced fabric with bath 3 3–4 4–5 4 5–6
relatively heavier coating on the fibre surface, which hindered move­ 4 4 4 4 6
ment of yarns within fabric hence a reduced extensibility. Meanwhile,
an increase in fabric extensibility is seen for fabrics mordanted in ul­
3.4. Functional properties of dyed cotton fabrics
trasonic bath and magnetic stirring bath, especially in ultrasonic bath
where 10% of extension gain is achieved. Ultrasonic irradiation and
3.4.1. UV protection
stirring induced turbulent flow are responsible for the observation.
UV index of dyed fabrics (soy concentration of 2–4%) are displayed
When fibers and yarns are relaxed in heated water and under external
in Table 3. The high transmittance values of UVA (10.43), UVB (8.75)
shock waves, they tend to be crimped more and form a bulkier and
and low UPF (Ultraviolet Protection Factor) value of 9.3 for control
loosened weaving structure, which then result in an increase in fabric
sample is regarded as poor. Application of FAA natural dye with soy
extensibility.
mordanting has improved UV protection to a large extent. It is seen that
the transmittance in both UVA and UVB region of ultraviolet spectrum
3.3. Color fastness of dyed fabrics
for dyed fabric has reduced and UPF increased dramatically in all cases.
Fig. 8 shows a bigger spectrum of fabric UPF values as a function of soy
Dyed fabrics with applicable soy mordant concentrations of 2–4%
mordanting. It is seen that regardless mordanting bath, UPF values
were investigated for Color fastness, and results are shown in Table 2.
increased with increasing soy concentration. This is expected as level of
It is seen from Table 2 that wash fastness and rub fastness of dyed
UV protection can be proportionally correlated to the color strength of
samples are at a rating range of 3–4 and 4–5, which is considered as good
fabrics (Riva et al., 2009; Alebeid and Zhao, 2017). An increase in
to excellent in grade, and meet the industrial scale. Light fastness are in
mordant content can result in an increased color strength (K/S) of the
rating range of 5–7 for all the samples tested, which is satisfactory for
dyeing from natural dye. Samples processed with ultrasonic has seen
slightly improved light fastness from that of water bath and magnetic Table 3
stirring bath, at soy concentration of 4%. These results indicate that the UV index of cotton dyed fabrics (mordant concentration of 2–4%).
connection between dye and cellulose through soy protein mordanting sample UV index
(Fig. 3) has been effective.
transmittance UPF grade

mordanting bath soy concentration T T

type (%) (UVA) (UVB)

control 10.43 8.75 9.3 poor

water bath 2 0.90 0.78 108.4 excellent
Table 1 3 0.73 0.65 127.4 excellent
Percentage strength loss and extension gain for 3% soy mordant dyed sample, 4 0.65 0.55 153.9 excellent
relative to the control sample (without mordanting). ultrasonic bath 2 0.64 0.53 160.1 excellent
3 0.54 0.45 192.8 excellent
sample ID (mordanting bath type) strength loss (%) extension gain (%)
4 0.51 0.42 201.3 excellent
water bath 5.42 − 6.26 magnetic stirring 2 0.64 0.55 153.4 excellent
ultrasonic bath 4.22 10.27 bath 3 0.56 0.48 172.8 excellent
magnetic stirring bath 4.60 7.23 4 0.55 0.45 187.5 excellent

6
Y. Zhang et al.
Fig. 8. UPF values vs soy concentration in various mordanting baths.
samples (Fig. 2), leading to an increased UPF values for soy mordant
dyed fabrics.
It is seen from Fig. 8 that the highest values of UPF were achieved
from ultrasonic bath when soy concentration exceeded 3%, which was
then followed by magnetic stirring bath and water bath. This could be
due to the accelerated and enhanced interactions between dye and fabric
surface as a result of ultrasonic irradiation and stirring. As has proven
previously, ultrasonic cavitation facilitated diffusion of dye into the fi­
bers. A significantly increased fabric dye intensity thus led to a higher
UV protection level (Sarkar, 2004; Zhang et al., 2022).
3.4.2. Antibacterial activity
Dyed fabric samples (at mordanting concentration of 3%) were
measured for antibacterial property, and the calculated results relative
to the control sample are displayed in Fig. 9. It is seen that for both E.
coli and S. aureus used in this work, all dyed fabrics have shown sig­
nificant improvement in bactericidal rate from the control sample. In E.
coli testing, percentage antibacterial activity is found to be higher with
sample mordanted in water bath than that of ultrasonic bath. This could
be due to the fact that in water bath, bio dye attracted by soy protein was
mainly settled on fiber surface, as has been proven previously in SEM
analysis (Fig. 5b) and fabric percentage weight increase measurement
(Fig. 7a). Greater surface area of soy coating (Fig. 5b) can then provide a
better chance for bio dye to get in touch with the bacteria. Whereas in
ultrasonic bath, parts of mordant/dye were diffused into fibers,
Fig. 9. Images and percentage antibacterial activity (against E. coli and S. aureus) of dyed fabrics from different mordanting baths.
7
Journal of Cleaner Production 336 (2022) 130465
therefore less bio dye was presented on the fiber surface to fight against
bacteria when compared with that of water bath.
A more effective bactericidal rate is seen achieved on S. aureus with
bactericidal rate of above 95% observed in all cases. The strong anti­
bacterial activity can be attributed to pharmacological activities of the
origin of FAA extracts. It is shown in previous studies that FAA extracts
can have broad spectrum antibacterial activity, and is particularly
effective in killing S. aureus (Chen et al., 2014; Zhao et al., 2008). Bio
dye from FAA was so powerful fighting against S. aureus that samples
mordanted in ultrasonic bath and magnetic stirring bath are showing a
complete bacteria removal rate of 100%. These results indicate that in
addition to the increased dye affinity provided to cotton fibers as a result
of soy mordanting, fabric bio function of antibacterial property can be
achieved simultaneously.
4. Conclusion
This study presented a green process of using ultrasonics and soy
protein mordanting to enhance cotton natural dye affinity and func­
tional finish with F. Artemisiae argyi (FAA) natural dye. Natural materials
with very little chemicals (no harm to the environment) were used in the
process. It is shown that fabric color strength (dye uptake) is increased
with increasing soy mordanting concentration, due to the effective
cellulose-soy-dye chemical interaction in the mordanting and dyeing
process. Ultrasonic bath is proven to be the most effective and efficient
mordanting bath among the three baths investigated. Ultrasonic assisted
mordanting can provide fabrics with higher color strength while
consuming less soy protein when compared with other mordanting
baths. Less weight increase as a result of ultrasonic irradiation can also
provide cotton fabric with softer handle than those processed in tradi­
tional water bath. Color fastness of dyed fabrics produced in this work
are within satisfactory level for industrial scale. UV protection of dyed
fabrics are found to be significantly improved from the control sample,
with ultrasonic mordanted samples showing the greatest improvement.
It is shown an outstanding anti S. aureus ability of dyed cotton in this
study, with bactericidal rate of 100% achieved at ultrasonics assisted 3%
soy mordant dyeing, owing to the inherent pharmacological properties
of FAA used as natural dye.
CRediT authorship contribution statement
Yanyun Zhang: Methodology, Investigation, Software, Writing –
original draft. Qi Zhou: Methodology, Investigation, Data curation.
Weibang Xia: Resources, Software. Luqman Jameel Rather: Method­
ology, Data curation. Qing Li: Supervision, Conceptualization, Writing –
review & editing, Project administration.
Y. Zhang et al. Journal of Cleaner Production 336 (2022) 130465

Declaration of competing interest different ph. Food Chem. 358, 129749. https://doi.org/10.1016/j.
foodchem.2021.129749.
McAdams, M.. Amino acids in soy protein. https://www.livestrong.com/article/35211
The authors declare that they have no known competing financial 7-amino-acids-in-soy-protein/ available in July 2021.
interests or personal relationships that could have appeared to influence Pan, Y., Hurren, C.J., Li, Q., 2018. Effect of sonochemical scouring on the surface
the work reported in this paper. morphologies, mechanical properties, and dyeing abilities of wool fibers. Ultrason.
Sonochem. 41, 227–233. https://doi.org/10.1016/j.ultsonch.2017.09.045.
Pisitsak, P., Hutakamol, J., Thongcharoen, R., Phokaew, P., Kanjanawan, K.,
Acknowledgement Saksaeng, N., 2016. Improving the dyeability of cotton with tannin-rich natural dye
through pretreatment with whey protein isolate. Ind. Crop. Prod. 79, 47–56. https://
doi.org/10.1016/j.indcrop.2015.10.043.
Support of this study from Chongqing Natural Science Foundation Pisitsak, P., Tungsombatvisit, N., Singhanu, K., 2018. Utilization of waste protein from
(project ID: cstc2018jcyjAX0493), and Fundamental Research Funds for Antarctic krill oil production and natural dye to impart durable UV-properties to
the Central Universities (project ID: SWU116040) are acknowledged by cotton textiles. J. Clean. Prod. 174, 1215–1223. https://doi.org/10.1016/j.
jclepro.2017.11.010.
the authors. Rather, L.J., Zhou, Q., Ali, A., Hague, Q.M.R., Li, Q., 2020. Valorization of natural dyes
extracted from Mugwort leaves (Folium artemisiae argyi) for wool fabric dyeing:
References optimization of extraction and dyeing processes with simultaneous coloration and
biofunctionalization. ACS Sustain. Chem. Eng. 8 (7), 2822–2834. https://doi.org/
10.1021/acssuschemeng.9b06928.
Adeel, S., Kiran, S., Habib, N., Hassan, A., Kamal, S., Qayyum, M.A., Tariq, K., 2019.
Rattanaphani, S., Chairat, M., Bremner, J.B., Rattanaphani, V., 2007. An adsorption and
Sustainable ultrasonic dyeing of wool using coconut coir extract. Textil. Res. J. 90
thermodynamic study of lac dyeing on cotton pretreated with chitosan. Dyes
(7–8), 744–756. https://doi.org/10.1177/0040517519878795.
Pigments 72 (1), 88–96. https://doi.org/10.1021/acssuschemeng.9b06928.
Adeel, S., Kiran, S., Yousaf, M.S., Habib, N., Hassan, A., Hassaan, M., 2021. Eco-friendly
Riva, A., Algaba, I., Pepio, M., Prieto, R., 2009. Modeling the effects of color on the UV
isolation of tannin based natural colorant from coconut coir (Cocos nucifera) for
protection provided by cotton woven fabrics dyed with azo dyestuffs. Ind. Eng.
dyeing of bio-mordanted wool fabric. Glob. NEST J. 23 (1), 65–72. https://doi.org/
Chem. Res. 48 (22), 9817–9822. https://doi.org/10.1021/ie9006694.
10.30955/gnj.003336.
Rym, M., Farouk, M., Bechir, E.M., 2016. Dyeing properties of cationized and non-
Alebeid, O.K., Zhao, T., 2017. Review on: developing UV protection for cotton fabric.
cationized cotton fabrics dyed with Vitis vinifera L. leaves extract. J. Text. Inst. 107
J. Text. Inst. 108 (12), 2027–2039. https://doi.org/10.1080/
(4), 525–530. https://doi.org/10.1080/00405000.2015.1046289.
00405000.2017.1311201.
Saleh, M.S., Abd, E.Y.A., Elbadry, K., 2019. Dyeing of cationized cotton fabrics with
Baig, U., Khatri, A., Ali, S., Sanbhal, N., Ishaque, F., Junejo, N., 2020. Ultrasound-assisted
natural dye extracted from Acacia. Chem. Cent. J. 7 (1), 1–24.
dyeing of cotton fabric with natural dye extracted from Marigold flower. J. Text.
Sarkar, A.K., 2004. An evaluation of UV protection imparted by cotton fabrics dyed with
Inst. 112 (5), 801–808. https://doi.org/10.1080/00405000.2020.1779907.
natural colorants. BMC Dermatol. 4 (1), 15. https://doi.org/10.1186/1471-5945-4-
Ben Ticha, M., Meksi, N., Drira, N., Kechida, M., Mhenni, M.F., 2013. A promising route
15.
to dye cotton by indigo with an ecological exhaustion process: a dyeing process
Suslick, K.S., 1989. The Chemical Affects of Ultrasound. Scientific American, pp. 80–86.
optimization based on a response surface methodology. Ind. Crop. Prod. 45,
Vankar, P.S., Shanker, R., Srivastava, J., 2007. Ultrasonic dyeing of cotton fabric with
350–358. https://doi.org/10.1016/j.indcrop.2013.02.009.
aqueous extract of Eclipta alba. Dyes Pigments 72 (1), 33–37. https://doi.org/
Chen, Y., Xu, W., Xu, S.Y., 2014. Germicidal effect of the leaves of Artemisia argyi
10.1016/j.dyepig.2005.07.013.
extract. J. Microbiol. 34 (6), 107–109 (Language in Chinese).
Wang, H., Memon, H., 2020. Cotton Science and Processing Technology - Gene, Ginning,
Eom, S.I., Shin, D.Y., Yoon, K.J., 2001. Improving the dyeability of natural colorants on
Garment and Green Recycling. Springer Nature Singapore Pte Ltd. https://doi.org/
cotton by cationization. Indian J. Fibre Text. Res. 26 (4), 425–431.
10.1007/978-981-15-9169-3. Published by.
Habib, N., Adeel, S., Ali, F., Amin, N., Khan, S.R., 2021. Environmental friendly
Xu, W.L., Li, Y., 2000. Cotton fabric strength loss from treatment with polycarboxylic
sustainable application of plant-based mordants for cotton dyeing using arjun bark-
acids for durable press performance. Textil. Res. J. 70 (11), 957–961. https://doi.
based natural colorant. Environ. Sci. Pollut. Res. 28, 54041–54047. https://doi.org/
org/10.1177/004051750007001104.
10.1007/s11356-021-14536-8.
Zhang, Y.Y., Zhou, Q., Rather, L.J., Li, Q., 2021. Agricultural waste of Eriobotrya
Haji, A., 2020. Plasma activation and chitosan attachment on cotton and wool for
japonica L. (Loquat) seeds and flora leaves as source of natural dye and bio-mordant
improvement of dyeability and fastness properties. Pigment Resin Technol. 49 (6),
for coloration and bio-functional finishing of wool textile. Ind. Crop. Prod. 169,
483–489. https://doi.org/10.1108/PRT-02-2020-0017.
113633. https://doi.org/10.1016/j.indcrop.2021.113633.
Janhom, S., Griffiths, P., Watanesk, R., Watanesk, S., 2004. Enhancement of lac dye
Zhang, Y.Y., Shahid-ul-Islam Rather, L.J., Li, Q., 2022. Recent advances in the surface
adsorption on cotton fibres by poly(ethyleneimine). Dyes Pigments 63 (3), 231–237.
modification strategies to improve functional finishing of cotton with natural
https://doi.org/10.1016/j.dyepig.2004.02.007.
colourants - a review. J. Clean. Prod. 335, 130313. https://doi.org/10.1016/j.
Kamel, M.M., El Zawahry, M.M., Ahmed, N.S.E., Abdelghaffar, F., 2009. Ultrasonic
jclepro.2021.130313, 2022.
dyeing of cationized cotton fabric with natural dye. Part 1: cationization of cotton
Zhao, N., Xin, Y., Zhang, C.L., 2008. Inhibitory effect of extracts from Artemisia argyi
using Solfix E. Ultrason. Sonochem. 16 (2), 243–249. https://doi.org/10.1016/j.
leaves on bacterial skin pathogenic bacteria. Chin. Herb. Med. 31 (1), 107–110
ultsonch.2008.08.001.
(Language in Chinese).
Lee, H.W., Lu, Y.Y., Zhang, Y.Y., Fu, C.L., Huang, D.J., 2021. Physicochemical and
functional properties of red lentil protein isolates from three different origins at