Bioactive and Multifunctional Wool Textiles Finish
Bioactive and Multifunctional Wool Textiles Finish
1, Article 3
Copyright ©2018-202, Rangsit University ISSN 2630-0656 (Online)
Cite this article: Chitichotpanya, P., Vuthiganond, N., Inprasit, T., & Chutasen, P. (2024). Bioactive and
multifunctional wool textiles finishing with Diospyros mollis Griff. extract. Journal of Current Science and
Technology, 14(1), Article 3. https://doi.org/10.59796/jcst.V14N1.2024.3
Bioactive and Multifunctional Wool Textiles Finishing with Diospyros mollis Griff. Extract
Abstract
Due to the sudden pandemic outbreak, there is a substantial demand for antimicrobial textiles for health and
hygiene. Natural dyeing with plant sources has been proven to be an excellent eco-friendly method for producing
healthcare textiles. In this study, Diospyros mollis Griff. extract was applied to the simultaneous dyeing and multi-
functionalization (antibacterial activity and UV-protection) of wool fabrics. Response surface methodology was applied
to optimize the treatment procedure and assess parameter interactions. The optimal result was achieved when dyeing at
pH 4, dye concentration 25 g/L, temperature 88°C, and time 95 min. The dyed fabrics had good antibacterial activity
against both E.coli and S.aureus (bacterial colony reduction > 90%), with E.coli being more pronounced. The UV
protection factor (UPF) also reached the maximum (40+) level, demonstrating their superior UV protection. The finished
wools are black, with high color strength (K/S > 9), good light and washing fastness, and fair to good crocking fastness.
Thus, Diospyros mollis Griff. fruit extract can be used as a new bioactive agent for multifunctional textiles, as well as
simultaneous black coloring.
Keywords: Diospyros mollis Griff; Wool; Functional textile; Antibacterial activity; UV-protection; Response surface
methodology
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Natural dyes are typically extracted with in Figure 1 (Yoshihira et al., 1971; Wang et al.,
water from their natural color sources (plants, 2018). Thus, Diospyros mollis Griff is a source of
microorganisms, animals, and minerals) (Nambela bioactive compounds that can be used as a natural
et al., 2020). These dyes can be used for coloration black quinone dye. Previous research shows that
of textile fibers, as well as other substrates such as natural quinone dye compounds are abundant,
hair, skin, paper, candle, and food. Some natural albeit in modest quantities, but all have the potential
dyes contain bioactive phytoconstituents that for increased production. In addition, they exhibit
impart functionalities to substrates such as insect superior dyeability, stability, brightness, and
repellent, deodorizing, antioxidant, antimicrobial, fastness in comparison to alternative natural dyes
and UV-protective properties, besides their like carotenoids and anthocyanins (Dulo et al.,
distinctive colors and tones (Chakraborty et al., 2021). However, it has received little attention as a
2020; Yemiş et al., 2022; Inprasit et al., 2018; source of plant dye to color or functionalize textile
Shabbir et al., 2018; Grifoni et al, 2020). Based materials. According to our review of the scientific
on their chemical structure, natural dyes can be literature, few studies have been conducted on the
categorized as carotenoids, quinoids, use of Diospyros mollis Griff. extract in textile
flavonoids, indigoids, tannins, pyridine-based, dyeing. (Thi et al., 2016; Phuong, 2020). In
and dihydropyrans (Mansour, 2018). The most addition, no studies have been conducted on the
prevalent natural dyes are the carotenoids, quinoids, fruit extract of Diospyros mollis Griff. as a
flavonoids. Of these, the carotenoids and flavonoids functionalization agent for antibacterial activity
have received the most attention. Polyphenolic and/or UV protection in wool textiles.
compounds, flavonoids, flavones, and tannins from The expanding market for medical and
plant dyes have been shown to absorb visible light healthcare textiles has created numerous
and UVB, thereby reducing their transmission opportunities for the use of natural colorants to
through substrates (Grifoni et al., 2020; impart functional finishes. The use of natural dyes
Vuthiganond et al., 2020). Additionally, natural to impart UV protection or antibacterial activity has
dyes containing polyphenols and phenolic been reported in literature (Chakraborty et al., 2020;
compounds can be considered as broad-spectrum Yemiş et al., 2022; Inprasit et al., 2018, Inprasit et
antibacterial agents (Baseri, 2022; Inprasit et al., al., 2020; Pisitsak et al., 2018; Sadeghi-Kiakhani et
2018; Inprasit et al., 2020). In recent years, al., 2021; Agnhage et al., 2017; Vuthiganond et al.,
numerous efforts have been devoted to identifying 2020). This study aims to promote the use of
new sources of natural dyes, reintroduce traditional Diospyros mollis Griff., a provincial tree in
natural dyes into modern dyeing practices, optimize Suphanburi Province, in functional textile dyeing
process conditions for their application, modify through a scientific approach. In the present study,
application methods, and enhance dyeing efficiency we hypothesized that Diospyros mollis Griff. fruit
(Nambela et al., 2020; Shahid & Mohammad, 2013; extract would act as a source of bioactive dye for
Haji, & Naebe, 2020). coloration, antibacterial activity, and UV protection
Diospyros mollis Griff., known as 'Makleua' on wool fibers due to the chemical composition of
in Thai, has been used as a medicinal plant for diospyrol. To achieve the desired results, natural
centuries. It belongs to the family Ebenaceae and is dyeing requires a delicate balance of treatment
predominantly cultivated in Southeast Asian conditions and application techniques (Alebeid et
countries. Its fruit extract contains a readily al., 2020). Optimization of process variables is one
oxidizable phenolic compound known as diospyrol of the crucial techniques for advancing the natural
(C 22 H 18 O 4 ), or tetrahydroxyl dimethyl bi- dyeing process. Hence, the response surface
naphthalene (Yoshihira et al., 1971; Suwama et al., methodology (RSM) in conjunction with Box-
2018), which has been used as an anthelmintic and Behnken design (BBD) was used to investigate the
a traditional black dye for silks. Diospyrol is significant effects of dyeing process factors (pH,
susceptible to air oxidation, and consequently, it dye concentration, temperature, and time) on color
turns black when exposed to air. The formation of strength of dyed wool fabrics. RSM has proven to
the black colorant is involved polymerization due to be a useful method for determining an appropriate
phenol radical coupling, quinone-phenol set of operational factors for optimizing the dyeing
rearrangement, and the formation of a phenol- process (Shahid et al., 2017; Sinha et al., 2016; Haji,
quinone charge-transfer complex, as demonstrated 2020; Yu et al., 2019; Haji, & Rahimi, 2020).
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2.2.5 Color measurement and fastness properties The average transmittance values in the UV-
The color coordinates and color strength A and UV-B zones are represented by Equation (6)
(K/S) values of the dyed wool fabrics were and Equation (7), respectively.
measured with a spectrophotometer (GretagMac
beth LLC, Switzerland) with illuminant D65, 10o ∑400 nm
315 nm Tλ ∆λ
T(UV-A)AV = ∑400 nm (6)
standard observer, and specular included. Each 315 nm ∆λ
measurement was done three times, and the mean ∑315 nm
290 nm Tλ ∆λ
values were complied. Using the Kubelka-Munk T(UV-B)AV = ∑315 nm (7)
290 nm ∆λ
equation, as shown in Equation (2), the K/S values
were calculated: 2.2.7 Antibacterial activity testing
The treated and untreated wool fabrics were
K (1-R)² assessed for their antibacterial activity against
S
= 2R (2)
Gram-positive S.aureus (ATCC 6538) and of
Gram-negative E.coli (ATCC 25922) by both
where K represents the absorption coefficient, S the qualitative and quantitative test methods.
scattering coefficient, and R the reflectance at Qualitative assessment was conducted by an agar
maximum absorption wavelength. diffusion method following AATCC Test Method
The color coordinates are expressed using 147. The test samples were cut into 6-mm-diameter
CIELab color space (L*, a*, b*), with L* discs and sterilized by exposing each side to 30 min of
corresponding to brightness (100 = white, 0 = UV radiation. 24 h broth cultures of test organisms
black), a* to red-green coordinate (+ve = red, -ve = (S.aureus and E.coli) were used as inoculums. The
green), and b* to yellow-blue coordinate (+ve = test organisms (1 x 105 CFU/ml) were dispersed
yellow, -ve = blue). C* value corresponding to throughout the surface of the agar plate and allowed
chroma and ho value to hue angle are computed to dry. The test sample was then meticulously put
using Equation (3) and Equation (4), respectively. on the agar plate alongside the tetracycline
antibiotics that served as the positive control. The
C* = [(a*)2 + (b*)2]1/2 (3) agar plates were incubated for 24 hours at 37 °C.
After incubation, the inhibitory effectiveness of the
ho = arctan(b*/ a*) (4) tested samples on the growth of the bacteria was
determined by measuring the diameter of the clear
Color fastness to light, crocking, and zone.
washing were assessed following ISO 105- A quantitative evaluation on the antibacterial
B02:1994, AATCC Test Methods 8-2013, and activity was conducted using AATCC Test Method
AATCC Test Methods 61-2013, respectively. 100. The test fabric was cut into 4.8 cm in diameter
circular swatches and sterilized by exposing each
2.2.6 Evaluation of UV protection side to 30 min of UV radiation. As a dilution
The UV protection property of untreated and medium and neutralizing solution, sterile normal
dyed fabrics was quantified via the measurement of saline was utilized. Circular test samples were
the Ultraviolet Protection Factor (UPF) using a inoculated with 1.0 mL of inoculums containing
CamSpec Spectrophotometer (Spectronic CamSpec either 1 x 105 CFU of E.coli or 1 x 105 CFU of
Ltd, England) in accordance with AS/NZS S.aureus. After incubation for 24 h at 37 °C, the
4399:1996. The UPF value was calculated from the percentage reduction (R) in colony numbers in the
total spectral transmittance using Equation (5): treated samples relative to the untreated sample was
calculated using Equation (6):
∑400 nm
290 nm Eλ Sλ ∆λ
UPF = 400 nm (5)
∑290 nm Eλ Sλ Tλ ∆λ R (%) = (B-A)/B х 100 (6)
where Sλ is the solar spectral irradiance, Eλ is the where R is the percentage reduction in bacterial
relative erythemal spectral effectiveness, Tλ is the colonies, A is the number of bacterial colonies from
measured average spectral transmittance of the treated fabric swatch after 24 hours of incubation,
specimen and ∆λ is the measured wavelength and B is the number of bacterial colonies from the
interval (nm). untreated sample before incubation.
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3. Results and Discussion Model terms with p-values larger than 0.05 are
3.1 Absorbance of the aqueous extract of considered insignificant and are removed from
Diospyros mollis Griff. the final model. The correlation coefficient (R2)
Figure 4 displays an UV absorption measures the quality of the model fit, and the p-
spectrum from 200 to 500 nm of aqueous Diospyros value confirms its statistical significance. The
mollis Griff. fruit extract. The UV radiation mainly closer R2 gets to 1, the better the model fits. If the
include UV-A band (315-400 nm), UV-B band p-value of the regression model is less than 5% (p <
(290-315 nm), and UV-C band (200-290 nm). In the 0.05), it is accepted. If this is not the case, the p-
upper atmosphere, oxygen and ozone absorb the value for lack of fit is more than 0.05. In this
high-energy UV-C spectrum. Approximately 95% investigation, the predicted model had an R2 of
of the solar UV radiation that reaches the earth 0.9554, indicating that it could only explain 4% of
surface is UV-B, whereas only 5% is UV-A (Rivas the variation. The anticipated R2 represents a
et al., 2020). UV-A causes little visible skin regression model's predicting accuracy for new
reaction and reduces the immune response of skin trials. The adjusted R2 is a modified form of the R2
cells, whereas UV-B is the primary cause of skin used to examine the predictive power of models
cancer development (Mongkholrattanasit et al., with different number of variables. The model is
2014). From Figure 4, it can be seen that the extract considered accurate if the difference between
can absorb radiation in the UV-C, UV-B, and UV- adjusted R2 and predicted R2 is less than 0.2 (Shahid
A regions. It can be suggested that absorption in the et al., 2017). The adjusted R2 and predicted R2
UV-B area could offer sufficient protection against values in this study are 0.8782 and 0.7824,
harmful UV rays. respectively. Furthermore, the F-value of the model
(148.35) with a low probability value (p < 0.05)
3.2 Regression analysis suggests that the model was statistically significant;
Table 2 presents the experimental outcomes consequently, the experimental values agree well
of BBD with three levels and four variables. The with the projected values, confirming the model's
K/S is the response or dependent variable, while the good predictability. It is possible to conclude that
independent variables were the dyebath pH, dye the produced model has a good level of
concentration, temperature, and time. The data was predictability within the given variable range.
then analyzed, and a quadratic regression model Table 4 shows the linear coefficients (A, B,
produced the following equation. The considered C, and D), quadratic coefficients (A2, B2, C2, and
response or dependent variable was the K/S, while D2), and interaction coefficients (AD and BC) are
the independent variables were the pH of the dye significant with p < 0.05. The coefficients of the
bath, dye concentration, dyeing temperature, and other terms are not significant (p > 0.05). As a
dyeing time. Then, the results were analyzed, and a result, A, B, C, D, A2, B2, C2, D2, AD, and BC play
quadratic regression model yielded the following important roles in defining the K/S values of dyed
equation: wool materials. Within the boundaries of the
experimental variables, the ANOVA analysis
K/S = -5.79 + 1.418*A + 0.279*B + 0.051*C + reveals that the model equation for the color
0.114*D - 0.27*A2 - 0.009*B2 - 0.001*C2 - strength of dyed wool fabrics using Diospyros
0.001*D2 + 0.007*A*B + 0.004*A*C + mollis Griff. fruit extract during the dyeing process
0.003*A*D + 0.003*B*C is applicable. The main, square, and interaction
where A denotes the dyebath pH, B the dye effects of independent variables are all significant,
concentration, C the temperature, and D the time. according to a regression analysis of the model
An ANOVA (Table 3) was used to determine equation.
the statistical significance of the BBD model.
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3.3 Effect of dyeing conditions on color strength molecules composed of hydroxyl groups (-OH)
The effects of pH, dye concentration, attain more negative charges as the pH increases.
temperature, and time on color strength of the Wool fiber would gain more negative charges when
dyeing process were investigated. The contour increasing the pH due to the ionization of
and response surface plots shown in Figure 6 carboxylic acid groups (-COOH) in wool structure
were created to analyze the interaction between (Figure 5). Thus, increasing the dyebath pH
the various independent variables and their increased the repulsive forces between the dye
corresponding effect on the response. As shown in molecules and the wool fibers, resulting in
Figure 6 (a, b, and c), the K/S values of dyed wool decreased dye absorption and K/S value in the dyed
fabrics decreased as the pH of the dye solution fabrics at higher pH values. Haji et al. demonstrated
increased. Observations indicate that the optimal that an increase in pH neutralizes the positive
values are obtained at pH 4. Changes in the charge of amino groups in wool, resulting in
chemical structure of dye molecules and wool fibers reduced electrostatic interactions and consequently
at different pH values have a significant impact on decreased dye adsorption on wool fibers (Haji, &
the adsorption of dyes on wool surface. Dye Rahimi, 2020).
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Both pH and temperature play important fiber reaches the saturation mode, the desorption
roles in natural dyeing processes and are regarded rate increases, leading to decreased K/S values.
as the most influential factors on dye binding to
fiber surface (Shahid et al., 2017). The response 3.4 Response Optimization and validation of the
surface plot (Figure 6 (b)) indicates a relationship model
between the pH and temperature of the dye solution Minitab's optimization function was utilized
in order to achieve the greatest color depth. At all to optimize the conditions for dyeing wool fabrics
temperatures, increasing the pH resulted in a with Diospyros mollis Griff. fruit extract. The
decrease in K/S values. optimization function examines a set of factor
Figure 6 (a, d, and e) represent the interactive levels that achieve the goal placed on response or
effect of dye concentration on pH, time, and dependent variable. In this study, the dyeing
temperature. The color strength gradually increased condition with the highest K/S value was selected
as the dye concentration increased from 15 to 25 from the provided range. As a result, Table 5 shows
g/L. This is because increasing the concentration of the proposed optimum conditions for wool fabric
the dye in the solution enhances the absorption of dyeing with natural dye extract. Indeed, the
experimental K/S value was 9.81, compared to the
dye molecules by the wool fibers. However, in a
predicted value of 10.65. As a result, the model
high dye concentration range, the increase in color
suggested in this study has been confirmed and
strength with increasing dye concentration was
validated. As a result, the optimal dyeing condition
substantially reduced, possibly due to the decreased was applied to dye fabric samples for evaluating
dyeing sites of wool fibers. This is a common their color fastness and UV protection properties.
phenomenon in dyeing processes. The effect of
dyeing temperature and time on K/S values was 3.5 Color Fastness Testing
more noticeable at higher dye concentrations. The dyeing of wool fabrics with Diospyros
Figure 6 (b, d, and f) represent the interactive mollis Griff. fruit extract yielded grey-black shade.
effect of dyeing temperature on pH, dye As shown in Table 2, the dyed samples' color data
concentration, and time. They show that the matched their visual appearance, as the color data
percentage of dye uptake increases with dye with low positive values of a* and b* were located
temperature and reaches a maximum at around 89 °C. in the red-yellow coordinate of the CIELab color
This could be due to the higher kinetic energy of the space. Color fastness is the capacity of a colored
dye molecules and the fiber swelling effect, both of textile to retain its original hue under normal
which enhance the dyeing capacity of the wool conditions of use, and it is a requirement for all
fibers. Furthermore, the dye solution contains single commercially dyed products. The degree of color
molecules as well as aggregates. Larger aggregates change determines the colorfastness. The washing,
reduce diffusion rates and surface adsorption, light, and crocking colorfastness of wool fabrics
lowering color strength and fastness. Increased dyed under the optimal conditions of this study are
temperature typically allows aggregates to disperse displayed in Tables 6-7. The color change value
while also increasing dye exhaustion and color was rated as 4 (good). A color staining test was used
strength, resulting in complete and uniform dying to further assess color stability. Table 6 shows the
(Baig et al., 2020). Higher dyeing temperatures degree of color staining on multifiber No.10
(above 89°C) reduce K/S values because the (acetate, acrylic, cotton, nylon, polyester, and
desorption rate of dye molecules may become wool). Each fiber in the multifiber fabric test has
greater than adsorption at such temperatures polar end groups such as hydroxyl (-OH) or amino
(Shahid et al., 2017). (-NH2) groups. As they leaked from the dye
Figure 6 (c, e, and f) represent the interactive samples and contaminated the test medium, these
effect of dyeing time on pH, dye concentration, and may interact with the phenolic and hydroxyl groups
temperature. As can be seen, the dye uptake by of the dye molecules via hydrogen bond
wool fibers was depended on time. Color strength interactions. All of the color staining values in
increased at initially, then fell, with the highest K/S multifiber fabrics were rated as good to excellent
value occurring in the middle of the dyeing process. (4-5) or good (4). As shown in Table 7, the dyed
This could be because the dye molecules were fabrics have good color fastness to crocking (rated
rapidly adsorbed at first due to the abundance of 4) in the dry state but fair to good (rated 3-4) in the
dyeing sites, but as the amount of dye fixed to the
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wet state. As predicted, the application of a polar property of the dyed fabric is evaluated as good
solvent increased the vulnerability of fabrics to when the UV transmittance is less than 5%. UPF
color loss upon rubbing, notably when wet. The values and percent transmittance of UV-A (315-400
dyed fabric's color fastness to light was also good nm) and UV-B (290-315 nm) radiations of
(rated 6). In conclusion, all of the fastness untreated and wool fabrics dyed under the optimal
properties were rated as good, indicating that this conditions were calculated and presented in Table
natural dye can be used to dye wools with high color 9. The results demonstrate a significant difference
strength as well as satisfactory color fastness. between the untreated and dyed wool fabrics. The
untreated wool fabrics had a low UPF of 6.24,
3.7 UV protection performance resulting in inadequate skin UV protection. As the
Proper UV rays are beneficial to the human dyed wool fabrics comprise functional groups that
body since they sterilize and stimulate vitamin D absorb UV radiation, they offer superior UV
synthesis. However, overexposure of skin to UV protection than the untreated wool fabrics, as
radiations can cause skin damage and even skin indicated by the higher UPF values and lower UV
cancer (Rivas et al., 2020). transmission percentage (Table 9). The UPF of the
UV protective textiles are becoming dyed wool fabrics also reached the highest (40+)
increasingly popular because they provide simple level, demonstrating the enhancing UV protection
and convenient UV radiation protection. The degree of the dyed wools.
of UV protection depends on a variety of factors
such as (1) type of fiber (most natural fibers offer 3.8 Antibacterial Activity
little protection), (2) fabric construction (thicker Wool fibers have a high surface-to-volume
and denser fabrics offer greater UV protection), (3) ratio and the ability to retain moisture, which is
fabric preparation (unbleached fabrics offer greater conducive to the growth of microorganisms
UV protection than desired and bleached fabrics), (Alebeid et al., 2020). Figure 8 depicts the
and (4) fabric's color strength (darker colors antibacterial activity against two key strains of wool
increase UV protection) (Vuthiganond et al., 2020). fabrics dyed under optimum condition. Firstly, the
Special UV protection coatings, such as the addition dyed fabrics were tested against S.aureus (Gram-
of optical brightening agents or UV absorbers, or positive) and E.Coli (Gram-negative) following
plasma treatment with nitrogen or silver, may be AATCC 147. Figure 7 shows the clear zone of
applied. (Ayesh et al., 2022; Shahidi, 2014). inhibition caused by untreated fabrics, dyed fabrics,
Wool fabrics offer insufficient UV and tetracycline antibiotics. The dyed fabrics were
protection because their fiber structure lacks superior to the untreated fabrics at preventing the
carbon-carbon double bonds or UV-absorbing growth of microorganisms, despite the fact that
molecules. Some natural dyes with an aromatic ring tetracycline had a more potent impact. The
or a highly polymerized polyphenol structure may antibacterial activity was then quantified and
function as UV absorbers and provide enhanced UV calculated as a percentage reduction following the
protection (Pisitsak et al., 2016; Vuthiganond et al., AATCC 100 method as shown in Figure 8. The
2020). To investigate the UV protection property of antibacterial reduction of the dyed wool fabrics
wool fabrics dyed under optimum condition, UPF against S.aureus and E.Coli was 90.65% and
and UV transmittance parameters are utilized to 93.64%, respectively. Although the dyed fabrics
determine the UV protection efficiency. The showed good antibacterial activity against both
percentage transmittance in UV regions measures bacteria, the effect was more pronounced against E.
the amount of UV rays that penetrate the skin and coli. Due to the interaction between the positively-
their effects, whereas the UPF rating system charged diospyrol and the negatively-charged
measures how well a fabric protects the skin from bacteria at the cell surface, the antibacterial activity
UV rays. According to the AS/NZS 4399:1996 test of the dyed sample is greater than that of the
method, textile products with a UPF value in the untreated sample. This interaction causes extensive
range 15-24 have “Good UV Protection”, 25-39 changes on the cell surface, leading to cell
have “Very Good UV Protection”, and 40-50+ have permeability (Fareed et al., 2022).
“Excellent UV protection”. Also, the UV protection
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Table 7 Color fastness to light (ISO 105-B02:1994) and crocking (AATCC 8-2013)
Crocking
Fastness to Light
Dry Wet
Dyed fabrics 6 4 3
Figure 7 Qualitative analysis for antibacterial activity (AATCC 147): (a) E.coli and (b) S.aureus
Figure 8 Quantitative analysis for antibacterial activity (AATCC 100): (a) E.coli and (b) S.aureus
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