http://pubs.acs.org/journal/acsodf

ArticleRapid Probing of Self-Cleaning Activity on Polyester Coated by
Titania−Natural Silica Nanocomposite Using Digital Image-BasedColorimetry
Diana R. Eddy,* Annisa Luthfiah, Muhamad D. Permana, Yusi Deawati, M. Lutfi Firdaus, Iman Rahayu,
and Yasuo Izumi

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ABSTRACT: Titania−silica nanocomposites (TiO2−SiO2) show outstanding performance and is very well applied in photocatalysis. In thisresearch, SiO2 extracted from Bengkulu beach sand will be used as asupporting material of the TiO2 photocatalyst for application to polyester
fabrics. TiO2−SiO2 nanocomposite photocatalysts were synthesized using
the sonochemical method. The coating of the TiO2−SiO2 material onpolyester was carried out using the sol−gel-assisted sonochemistry
method. The method of determining self-cleaning activity uses a digital
image-based colorimetric (DIC) method, which is much simpler thanusing an analytical instrument. The scanning electron microscopy−energy
dispersive X-ray spectroscopy results showed that the sample particles
adhered to the fabric surface and the best particle distribution was shownin pure SiO2 and 1:0.5 TiO2−SiO2 nanocomposites. Analysis of Fouriertransform infrared (FTIR) spectroscopy proved the presence of Ti−O and
Si−O bonds as well as the typical spectrum of polyester, which indicated that the fabric had been successfully coated with
nanocomposite particles. The analysis of the contact angle of the liquid on the polyester surface showed a significant change in theproperties of the TiO2 and SiO2 pure coated fabrics, but changes occur only slightly in the other samples. Self-cleaning activity
against the degradation of methylene blue dye has been successfully carried out using DIC measurement. The test results showedthat the best self-cleaning activity was shown by TiO2−SiO2 nanocomposite with a ratio of 1:0.5 with the degradation ratio reaching
96.8%. Furthermore, the self-cleaning property remains after the washing process, which shows excellent washing resistance.

■

INTRODUCTION
Recently, the application of nanoparticles to textiles is
becoming an extensive research topic worldwide.1 Textiles
are flexible materials made from interlocking bundles of yarn or
yarn, produced by spinning raw fibers.2 One type of textile thatis widely used is polyester fabric. This fabric is a type ofsynthetic fabric that is strong, durable, and does not wrinkle.
Polyester fabrics are often used in the manufacture ofsportswear, underwear, bed linen, and medical clothing.3
This type of clothing needs to have sufficient quality ofresistance to dirt. Commercially, soiling substances on clothes
need to be removed by using detergents. However, excessive
use of detergents can cause various problems, such as
generating wastes that pollute the aquatic environment,4
cause poisoning in aquatic organisms,5 cause disease,1 andproduce water insufficient for consumption.6 One of the efforts
that can be done to minimize the use of detergents is to bringup self-cleaning properties on the surface of textile fabrics.
Self-cleaning in the fabric is one of the characteristics that
attracts the attention of the textile industry.7 This property
maintains the clean condition of the fabric resulting to protect© 2023 The Authors. Published byAmerican Chemical Society

the body from dirt and reducing the amount of use of chemical
disinfectants.8 Modification of textile surfaces by coating or
coating using certain materials is a simple and effective waythat can be done to bring out these properties. However, thefabric coating process needs to meet several requirements forthe functionalization of textiles including technologicalefficiency, high stability against washing, inexpensive cost,
and the utilization of nontoxic materials.9 Several methods ofcoating self-cleaning materials on fabrics have been carried out
such as sol−gel, sputtering, electrochemical, and spraying.10
Among these technologies, the sol−gel-assisted sonochemistrybased coating method is known to meet the requirement for
the functionalization of all kinds of textiles.11 Ultrasonic
Received: November 28, 2022
Accepted: February 3, 2023
Published: February 15, 2023

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ArticleTable 1. Variation of Samples Coat Polyester Fabrica
samplefillersample code

TiO2
natural SiO2
NC-TS-1:0.5
NC-TS-1:1
NC-TS-1:2

P
P-TiO2P-SiO2
P-TS1:0.5
P-TS1:1
P-TS1:2

polyester 30 × 30 cm2

mass (mg)volume H2O (mL)volume C2H5OH (mL)volume HCl (mL)

58
58
58
58
58

0.5
0.5
0.5
0.5
0.5

without treatment
42
42
42
42
42

100
100
100

a

NC-TS = TiO2-SiO2 nanocomposite. P-TS = Polyester coated TiO2-SiO2 nanocomposite.

showed selective adsorption and good photocatalytic activity.24
The use of a natural SiO2 supporting material for the TiO2
photocatalyst has produced excellent results in the remediationof Cr(VI) and Pb(II) metals.25 Research related to thephotocatalytic activity and photo-induced superhydrophilicity
of TiO2−SiO2 nanocomposites as well as their characterizationon the molecular level has been reported.26−28 In our previous
work, the TiO2 photocatalyst has been successfully combinedwith natural SiO2 supporting material from beach sand and has
produced better photocatalytic performance than TiO2
alone.29 Based on this context, this study focuses on thesustainable use of titania−natural silica nanocomposite(TiO2−SiO2) as a functional material for coating polyester
fabrics using the sol−gel assisted sonochemistry method in its
application as a self-cleaning cloth. The self-cleaning activity
test of MB dye on the fabric was analyzed using a simpler
renewable calorimetry analysis, namely, the image-based
colorimetry method.

radiation in the liquid causes the process of acoustic cavitation,
namely, the formation, growth, and collapse of bubbles
implosively.12 Under these conditions, chemical reactions
occur and new products are created very quickly andefficiently. Thus, the process becomes faster and can produce
the expected product.
One of the appropriate materials that enable self-cleaning
properties on fabrics is the metal oxide photocatalystmaterial.13 Photocatalytic activity allows the material tointeract with the environment and produce the reactive oxygen
species (ROS).14 These species are able to decompose organic
pollutant compounds into simple inorganic compounds thatare finally removed from the living environment by the effectsof heat, wind, or rain.8 So far, metal oxide materials have been
proven to exhibit such properties on textile surfaces, including
water repellence, antibacterial activity, UV protection, and selfcleaning.15 One of the most widely used materials for selfcleaning applications is TiO2. This material is a semiconductormaterial that is widely applied as a photocatalyst.16 This isbecause TiO2 has many advantages such as high photocatalytic
activity, sufficient chemical stability, high oxidizing power, low
toxicity, and abundance on the earth.17,18
Various studies testing self-cleaning have been reported.
Methylene blue (MB) dye is often used as an example ofchemicals that needs to be removed for environmental
protection. These dyes have the characteristics of poor
biodegradability so they are suitable for self-cleaning testing.
A digital image-based colorimetry (DIC) method has beenutilized in this study for easier and simpler measurement of
substance concentration. This method can determine thesample concentration by referring to the dynamic range of thedigital image represented by the red−green−blue or RGB
color space (that is, from 0 to 255). This color space is muchwider than conventional colorimetric or spectrophotometricmethods (that is, from an absorbance of 0 to 2.0), thusincreasing the sensitivity of detection.19 The value of thesample concentration is obtained by following the equation,
resulting from the standard curve. This method is a promisingalternative new technique with various advantages. Firdaus etal. demonstrated several advantages of this method, such as theanalytical procedure, which is environmentally friendly,
inexpensive, portable, and simple to analyze various chemicalcompounds.20 This method is carried out with the help of the
ImageJ application to measure the red−green−blue (RGB)
color which is able to increase the detection sensitivity.21,22
Research studies conducted by Li et al.11 and Ojstršek andFakin23 has coated TiO2 nanoparticles with SiO2 synthesizedfrom TEOS precursors on polyester/cotton fabrics withrepeated washings, resulting in good washing durability andphotostability. The decolorization process of MB dye in thepresence of a photocatalyst was monitored under UV
illumination using synthetic TiO2 and TiO2/SiO2 which■

EXPERIMENTAL SECTION

Materials. The main material used in this study consistedof 100% white microfiber polyester fabric with a density of 30
threads/cm and a fabric weight of 108 g/m2 supplied by TJ
textile Co., Ltd. Titanium−silica nanocomposites (TiO2−
SiO2) were synthesized. Other supporting materials in thisstudy consist of distilled water (Merck), aquabides (Merck),hydrochloric acid (HCl, 37%, Merck), nonionic detergent(Tween 80), absolute ethanol (C2H5OH, 100%, Merck),
extract silica from beach sand (from Bengkulu, Indonesia),
methylene blue (Merck), and titanium dioxide (TiO2, P25
Degussa, Merck). All materials used are pro analysts.
Polyester Fabric Coating. The nanocomposite synthesis
method is the sol−gel assisted sonochemistry method that has
been reported in our previous study.29 In addition, theselection of variations, composition, and sample precursors arealso different from reference studies. The coating method on
the fabric using the sol−gel assisted sonochemistry methodrefers to the research method of Li et al.11 modified. Polyester
fabric is washed with a nonionic detergent at 50 and rinsed
using aquabides. The cloth was immersed in the ethanol−
water solvent with a volume ratio of 3:4. Then, the HCl
catalyst was added (Table 1) and sonicated. Sample variations
were added slowly and resonicated. Fabric was dried at 65 °C
for 2 h, then 80 °C for 5 min, and 120 °C for 3 min. The
procedure is repeated three times and then heated for 2 h at100. The variation of samples is shown in Table 1.
Polyester Fabric Characterization. Characterization
analysis on polyester fabric was carried out by the opticalangle test, SEM, and FTIR analysis. Analysis of the opticalangle test was carried out with (Specification) functioned todetermine the contact angle on the fabric. The resulting data
will be used to determine the surface properties of the material.

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The distilled water is dripped at a distance of 1 cm from thesurface of the cloth. Next, the contact angle on the fabric wasdetermined. Scanning electron microscopy (SEM, Hitachi SU3500, Tokyo, Japan) analysis with a voltage of 3.00 kV at amagnification of 2000× was performed to determine thesurface morphology of the fabric. The photocatalysts were
further characterized using Fourier-transform infrared spectroscopy (FTIR, PerkinElmer Spectrum 100, Massachusetts,USA) to determine the functional groups in the composites. In
determining this performance, a solution of methylene blue
dye is needed, which is prepared with various concentrations of
30 and 300 ppm. The dye was then dripped one drop ofmethylene blue solution each vertically using a 1 cm burette ona cloth on a flat surface and allowed to stand for 3 min. The
cloth was then irradiated with a mercury lamp (HPL-N 125 W
Philips) at a distance of 10 cm and a sample image was taken
every 60 min for 6 h using a smartphone camera. Furthermore,
the percentage decrease in the dye concentration was
calculated using a calorimetry-based digital image method.
The camera Redmi Note 10 (Xiaomi Inc.), with thecharacteristics of Table 2, was used to record images forin each sample. Average RGB values were measured with the
ImageJ 1.52a (NIH Image) image processing toolbox (Figure
2).
Digital image retrieval and ImageJ sample processing werecarried out in three replicates. Further analysis of the RGB data
was performed by Excel 2019 (Microsoft Inc.) and Minitab 19
software (Minitab Inc.) for simple linear regression and partial
least squares, respectively. RGB color values are converted to alogarithmic scale to obtain color intensity, following theLambert−Beer law equation.30
Quantification of Digital Images. The average color
values of R, G, and B were analyzed using ImageJ 1.52a
software. A specific image area is selected. The RGB color
value is selected in a certain area consisting of several
important pixels to get accurate results. To obtain a linear
line for further simple uses, such as a standard calibration
curve, the initial RGB color value is converted to the intensity
obtained using Lambert−Beer’s law as follows (1):I(R,G,B) = log(A 0(R,G,B)/A s(R,G,B))

focal length
metering mode
image format
color representation
software for image
computation
RGB color measurement
image data processing(1)

I(R,G,B)is the effective intensity of the respective color, A0(R,G,B)
and As(R,G,B) are the red, green, and blue color values of theblank and sample, respectively. The digital camera functions asa spectrophotometer that analyzes light from methylene blue.
The intensity shown is the sum of the R, G, and B color valuesof the digital image.19,20
Washing Resistance Test. The endurance test methodrefers to the research method of Petkova et al.42 The cloth issoaked in distilled water. The cloth was shaken at 30 rpm for
15 min and dried.

Table 2. Characteristics of Digital Cameras
digital camera
camera maximum resolution
sensor size
pixel size
conditions to take pictures
exposure mode

ArticleRedmi Note 10, Xiaomi Inc.
48 megapixels
6.4 × 4.8 mm
0.8 μm
AI portrait mode with blur and depth control,
f/1.7926 mm
spot metering
JPEG, 2604 × 4624 pixels
sRGB (standard RGB)■RESULTS AND DISCUSSION
Scanning Electron Microscopy Analysis. The material
characteristics of TiO2−natural SiO2 nanoparticles have been
described in our previous study.29 SEM analysis at 2000×
magnification showed particle dispersion and sample agglomeration on the polyester fabric surface. Figure 3a shows thesmooth surface of the polyester fabric before coating with thesample. Meanwhile, the sample particles coated on the surfaceof the fabric form a rough surface which can be seen clearly in
Figure 3b−f.
Sonochemical TiO2 tends to aggregate and does not coatwell (Figure 3b).32 The particle size of TiO2 on the fabricsurface was significantly larger (mode range: 60−70 nm;
Figures 3b and 4a) than that of the natural SiO2 sample (moderange: 30−35 nm; Figure 3b). The reason is that only the SiO2
extraction process from sand goes through a top−downmethod based on the literature procedure.29 The porous
structure of SiO2 suited well for the dispersion on the fabricsurface especially when the ratio of TiO2 was greater comparedto SiO2 (Figure 3d−f), probably because relatively smaller
TiO2 nanoparticles were well filled in the pores of SiO2 during
the sol−gel synthesis of TiO2−SiO2 composites.
In clear contrast, Figure 3d shows good particle distribution
with minimal agglomeration. Meanwhile, P-TS1:1 still showedsome agglomerated particles and uneven coating (Figure 3e).
P-TS1:2 shows agglomeration that dominates with a fairly evencoating (Figure 3f). Luthfiah et al. showed the differences in
the particle size of each sample in the powder form.29 Figure
4c−e shows the increase in the particle size along with theaddition of natural SiO2 to the composite. This proves that the
samples coated tend to agglomerate at a larger powder particle

ImageJ 1.52a
Excel 2019, Minitab 19

viewing color-based digital images. ImageJ 1.52a (NIH image),
Excel 2019 (Microsoft Inc.), and Minitab 19 (Minitab Inc.)
were used for digital image data processing.
Digital Image Capture Method. The method ofdetermining the concentration of the dye on standard solution
fabrics and samples placed under constant ambient light andphotographic conditions (Figure 1). Details of camera settings
are shown in Table 2. Colors are obtained from thesurrounding representative circle region 1000 pixels locatedFigure 1. Shooting studio for the image to be captured RGB values.
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ArticleFigure 2. Sample operation using ImageJ 1.52a application.

Figure 3. SEM data of polyester fabric of sample (a) polyester (P); (b) P-TiO2; (c) P-SiO2; (d) P-TS1:0.5; (e) P-TS1:1; (f) P-TS1:2.

Figure 4. Result of the distribution size of particles in the polyester surface with (a) TiO2, (b) natural SiO2, (c) TiO2−SiO2 1:0.5, (d) TiO2−SiO2
1:1, (e) TiO2−SiO2 1:2.

size. Sonochemical TiO2−natural SiO2’s is relatively homogeneous size distribution and nicely coat on polyester.
Furthermore, TiO2 shows hydrophilic properties; thus, thecoating at the ratio TiO2−SiO2 of 1:0.5 was the best.
Sonochemistry involves administering ultrasonic waves which
produce an acoustic cavitation process. This method is capableof producing smaller particle sizes and more regular crystal
shapes.33
FTIR Analysis. FTIR analysis was carried out to identify thefunctional groups of the polyester fabric before and after thecoating process from TiO2−SiO2 with a molar ratio of 1:0.5;
1:1; and 1:2 in the wave number range of 500−3500 cm−1.31
Figure 5a shows the types of bonds in polyester fabrics in theform of C�O, C�C aromatic, and C�C bonds which arethought to indicate the presence of ester, alcohol, anhydride,
aromatic ring, and heterocyclic aromatic ring functionalgroups. Figure 5b shows absorption at a wave number of856 cm−1 which proves the existence of Ti−O bonds. While on
the sample, P-SiO2 (Figure 5c) shows a peak at thewavenumber 798 cm−1, which proves the existence of Si−O
bonds. In the sample of cloth coated with the TiO2−SiO27861

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The results show that the polyester fabric has hydrophobic
properties. This property needs to be maintained in selfcleaning applications because water can be a medium for
impurities to absorb into the fabric. The addition of silica to
the titania photocatalyst managed to maintain the hydrophilicity of the fabric and tended to increase. Meanwhile, theapplication of pure TiO2 and SiO2 to the fabric makes the
fabric superhydrophilic (Figure 6b,c). It was observed that thewater contact angle decreased drastically to zero after applying
pure TiO2 and SiO2 to the polyester fabric samples, resulting infast water absorption. Basically, the surface energy of solids ingeneral and of fabrics in particular is highly dependent on thesurface area and the intermolecular forces present on thesurface.35 The content of hydroxyl groups in pure samples canbe produced higher. This causes charge imbalance thatprovides Lewis acid sites, thereby absorbing more hydroxyl
groups on the surface of the photocatalyst.36 Several studies
have also revealed that nano-SiO2 is extremely hydrophilic dueto the presence of a large number of hydroxyl groups on its
surface. The higher density of silanol tends to make the surfacehydrophilic.37
In addition, the wettability behavior can be greatly
influenced by the formulation of the sample that is coatedon the fabric.38 This trend can be attributed to the increasing
number of Ti−O−Si physical bonds at the TiO2−SiO2
granular interface (Figure 6d−f). This is in line with theresearch of Houmard and Riassetto36 which explains thatinteractions at the granular TiO2−SiO2 interface can cause
certain wettability behaviors.39 In addition, according to De
Gennes et al.,38 morphological properties, such as surface
roughness or exposed porosity, affect the measurement of thewater contact angle by increasing the wettability of the water.
Then, the variety of composites synthesized showed that an
appropriate amount of TiO2 was able to fill the pores in SiO2
so that it was able to provide hydrophobic properties to thefabric layered material.40
Self-Cleaning Activity Tests. Standard Curve. The
accuracy of the proposed method was evaluated by replicating
the image capture analysis and RGB calculations of the same
sample. In addition, three tests were also carried out todetermine the accuracy of the measurement of methylene blue
degradation. The relative standard deviation (RSD) was
evaluated as 3.6 × 10−3, 2.1 × 10−3, and 1.4 × 10−3 for R,
G, and B, respectively. These results indicate a good
reproducibility of the proposed method.
The slope of the calibration curve is 1.46 × 10−4, 2.11 ×
10−4, and 2.23 × 10−4 for R, G, and B, respectively (Figure 7).
This shows that blue has the highest sensitivity compared to
red and green. This is because the transmitted color inmethylene blue is dominated by blue, which causes a larger andmore sensitive gradient slope.
The three colors of the resulting standard have good
linearity. Therefore, calculations were carried out to determine

Figure 5. FTIR spectrum of sample (a) P; (b) P-TiO2; (c) P-SiO2;(d) P-TS1:0.5; (e) P-TS1:1; (f) P-TS1:2.

nanocomposite (Figure 5d−f), there is a signal spectrum of
Si−O and Ti−O which proves that the sample contains these
two functional groups. Table 3 shows the wavenumbers of theTable 3. Wavenumber of the Sample
wavenumber (cm−1)
type of bondP

P-TiO2 P-SiO2 P-TS1:0.5 P-TS1:1

P-TS1:2

Csp2−H
Csp3−HC�O
C�CaromaticC�C
stretching
Ti−O
Si−O−H
Si−O

3063
2968
1731
1454

3069
2981
1712
1408

3070
2975
1717
1420

3063
2961
1717
1400

3056
2968
1724
1406

3063
2964
1709
1394

703

715

710

717

723

696

865

858

541

580

876
823
547

856
798
527

Articletypes of bonds present in the sample. It was found that the
sample was successfully coated on the surface of the polyester
fabric based on the Ti−O and/or Si−O stretching vibration
peaks.34
Fabric Surface Contact Angle. In this study, the watercontact angle of the coated sample was measured (Figure 6).

Figure 6. Contact angle of sample (a) P; (b) P-TiO2; (c) P-SiO2; (d) P-TS1:0:5; (e) P-TS1:1; (f) P-TS1:2.
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Articlepeak intensity change as a function of the concentration of MB
was obtained (Figure 8b). The results of the accuracy test are
shown in Table 5. The ratio was calculated using eq 4.
Ratio (%) = CDIC/CSpectro × 100%

where CDIC is the concentration of methylene blue calculatedusing a digital image and CSpectro is the concentration of
methylene blue calculated from a UV−Vis spectrophotometer.
The percentage ratio shows the accuracy of the concentration
analysis results using the DIC method with the commonlyused method, namely, UV/Vis spectrophotometry. From the
proposed digital image-based colorimetric method, theunivariate results gave 108.40%. Then, multivariate results
gave 97.17%. These results were close to 100% and showed thecloseness of the sample concentration values using the DIC
method compared to UV/vis spectrophotometry. Therefore,
this method has satisfactory accuracy and precision.
Methylene Blue Dye Degradation. The photodegradation
test using samples against methylene blue solution was carriedout using the DIC method. The activity time course trendusing samples with different MB concentrations gave similar
decomposition rate constant. This shows that self-cleaning was
effective even though there were a difference in theconcentration of the substance tested for the color. The C/
C0 value of the MB dye solution was plotted against time toobserve the degradation rate of MB, where C is theconcentration of the target dye solution at the irradiationinterval and C0 is the initial concentration of the dye. All
samples including negative control in the form of untreatedpolyester fabric still experienced a decrease in the concentration of MB. This is due to the effect of dye adsorption on
the polyester fabric which decreased the MB concentration.41
Self-cleaning properties of MB stains were tested with twoconcentration variations before and after being irradiated witha UV lamp for 6 h, as shown in Figures 9 and 10.
MB is relatively stable under UV lamp irradiation when only
a noncomposite substance is used to coat the polyester fabric.
The time course change using the untreated polyester (Figure
6a,b, black lines) was due to adsorption, and further deviation
using the TiO2−SiO2-treated polyester was due to photocatalysis. However, when MB was adsorbed on the nanocomposite-coated polyester fabric, MB decreased in concentration at different rates depending on the variation of themolar ratio used. It can be noted from the degradation curvethat the P-TS1:1 sample decreased the MB degradation rate.
The reason for the lower degradation rate of MB can be
attributed to the agglomeration at the active site of the sample,
as evidenced from the previous SEM analysis shown in Figure
3e. The results showed that the sample P-TS1:0.5 gave the best
results in the degradation of methylene blue. This result is
supported by an even distribution of particles and minimal
agglomeration in the SEM data and the ability of the sample tomaintain hydrophobic properties to optimize the self-cleaning
activity of the fabric. The decrease in stain concentration every
hour for 6 h is shown in Table 1S.
Washing Test Results on Fabric. As shown in Figure 11,
it is known that after the washing test in water at room
temperature for 15 min, polyester fabric that has been coatedwith the TiO2−SiO2 composite (1:0.5) still has gooddegradation activity, which is around 72 and 82% for MB
concentrations of 30 and 300 ppm, respectively. Meanwhile, inpure TiO2, there was a significant decrease which means thatthe bond between TiO2 and polyester fabric was not formed

Figure 7. Standard curve of the variation of methylene blue
concentration against RGB calculated using univariate simple linear
regression.

the effect of three variables R, G, and B on the concentration of
methylene blue. Simple linear regression provided the easiest
calculation. On the other hand, the partial least squares (PLS
regression) calculated using Minitab 19 software (MinitabInc.) was a better calculation method by treating RGB data as
multivariate, resulting in a new linear regression shown in eq 2.
The resulting equation has linearity which is good with acorrelation coefficient of 0.9974. The measurement ofsignificance was also carried out using this application bylooking at the p-value for each variable (Table 4). Thisequation was then applied to a sample of methylene blue thatwas degraded from the photocatalyst material that had beencoated to polyester.
(2)

Conc. = 5.75 + 2995 R + 1753 G + 854 B

Table 4. Average RGB Color Values of MB
color value

color intensity

conc. MB
(ppm)

R

G

B

R

G

B

0
50
100
150
200
250
300
350

106.30104.04102.57101.92
99.41
98.49
95.69
94.19

116.36114.83110.31
108.16106.74102.61102.4997.46

148.21140.44136.69131.01129.24128.40123.23123.02

0
0.009
0.015
0.018
0.029
0.030
0.045
0.052

0
0.005
0.023
0.032
0.037
0.054
0.055
0.077

0
0.023
0.035
0.053
0.059
0.062
0.080
0.081

RGB color value (A(R,G,B)) is obtained from ImageJ software
analysis. The color value is used to determine the color
intensity (I(R,G,B)) with eq 3.
I(R,G,B) = log(A 0(R,G,B)/A s(R,G,B))

(4)

(3)

I(R,G,B) are the ef fective intensity of the respective colors, A0(R,G,B)
and As(R,G,B) are the red, green, and blue color values of the blankand samples, respectively.
Validate Method. The DIC method was validated bycomparison with the UV/vis spectrophotometric method.
Using a UV−vis spectrophotometer, methylene blue showed amaximum peak at the wavelength of 665 nm (Figure 8a). The
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ArticleFigure 8. (a) Determination of the maximum wavelength of methylene blue (the samples for this study were diluted 100 times using mess flask andmess pipette for UV−visible measurements), (b) calibration curve of the external standard method.

Table 5. Comparison of the Concentration Evaluation MB Based on DIC and the Spectroscopy Method (n = 3)
univariate = blue

multivariate

concentration (ppm)

DIC (ppm)

ratio (%)

DIC (ppm)

ratio (%)

UV−vis spec. (ppm)

300

317.31 ± 3.07

109.49301.31 ± 4.87

96.20

289.79Figure 9. Decrease in the concentration of methylene blue with variations in concentrations of (a) 30 ppm and (b) 300 ppm.

Figure 10. Methylene blue stain on polyester fabric before and after irradiation for 6 h (a) P; (b) P-TiO2; (c) P-SiO2; (d) P-TS1:0:5; (e) P-TS1:1;
and (f) P-TS1:2.

strongly. On the other hand, SiO2 showed a slight decrease inactivity which means that the presence of SiO2 plays animportant role in strengthening the bond between thecomposite and the polyester fabric.42 However, the effect of7864

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ArticleFigure 11. Graph of decreasing degradation activity of methylene blue with concentration before and after the washing test to the fabric (a) 30
ppm and (b) 300 ppm.

■

the amount of SiO2 on the composite in the resistance towashing is different depending on the composition. The TS1:1
composite has the most minor decrease in activity after
washing compared to other compositions, showing asynergistic effect of TiO2 and SiO2 in bonding with thepolyester fabric.43,44 When the amount of SiO2 or TiO2 is an
imbalance in the composite, this synergistic effect tends todecrease evidenced by the decrease in activity after washing.
According to previous reports, hydrophilic SiO2 and TiO2
nanoparticles have many OH− groups which cause thenanoparticles to aggregate.45 Thus, the appropriate ratio of
nanoparticles will cause hydrophilic nanoparticles to form
microstructural aggregations, which can create strong bonds
with polyester fabrics which make it resistant to washing. In
addition, the effect of the amount of SiO2 on the composite inresistance to washing is different depending on thecomposition. The TS1:0.5 composite which has a small
amount of SiO2 provides the best resistance compared toTS1:2 composite which has more SiO2 than TiO2. The reason
is because of the high hydrophobicity of the TS1:0.5
composite, making it resistant to washing.

■

ASSOCIATED CONTENT* Supporting Information
sı

The Supporting Information is available free of charge athttps://pubs.acs.org/doi/10.1021/acsomega.2c07606.
Fabric on the color stain self-cleaning testing process
(PDF)

■

AUTHOR INFORMATION

Corresponding Author

Diana R. Eddy − Department of Chemistry, Padjadjaran
University, Sumedang 45363, Indonesia; orcid.org/00000002-8384-5978; Email: diana.rahmawati@unpad.ac.id
Authors

Annisa Luthfiah − Department of Chemistry, Padjadjaran
University, Sumedang 45363, Indonesia
Muhamad D. Permana − Department of Chemistry,
Padjadjaran University, Sumedang 45363, Indonesia; Centerfor Crystal Science and Technology, University of Yamanashi,
Kofu, Yamanashi 400-8511, Japan
Yusi Deawati − Department of Chemistry, Padjadjaran
University, Sumedang 45363, Indonesia
M. Lutfi Firdaus − Graduate School of Science Education,
University of Bengkulu, Bengkulu 38371, Indonesia
Iman Rahayu − Department of Chemistry, Padjadjaran
University, Sumedang 45363, Indonesia
Yasuo Izumi − Department of Chemistry, Graduate School of
Science, Chiba University, Chiba 263-8522, Japan;
orcid.org/0000-0001-8366-1864
Complete contact information is available at:https://pubs.acs.org/10.1021/acsomega.2c07606

CONCLUSIONS

The addition of natural silica to the titania photocatalyst
increases the distribution of particles evenly on the surface ofthe fabric in the process of coating or coating polyester fabrics
with the sol−gel-assisted sonochemistry method. However, theaddition of SiO2 with a ratio equal to or greater than the TiO2
photocatalyst increased the occurrence of agglomeration on
the surface, as seen from the SEM image. These results affectthe surface properties and the self-cleaning activity of thefabric. The success in the coating process is evidenced by thepresence of titania and silica bonds on the surface of the fabricbased on the results of FTIR data analysis. Nanocomposite
coatings on fabrics are able to maintain the hydrophobic
properties of polyester fabrics needed to support self-cleaning
activities. Tests in the degradation of dye stuffs gave significant
results reaching 96.8% and the test results after washing werequite good (not changed significantly).

Author Contributions

Conceptualization, D.R.E. and M.L.F.; methodology, A.L.;
software, A.L.; validation, D.R.E., M.L.F. and Y.I.; formal
analysis, A.L.; investigation, A.L.; resources, A.L.; data
curation, A.L.; writing original draft preparation, A.L.; writing,review, and editing, A.L., Y.D., D.R.E., M.L.F., M.D.P., and Y.I.;
visualization, M.D.P.; supervision, D.R.E., Y.D., M.L.F., andY.I.; project administration, D.R.E. and Y.I.; funding
acquisition, D.R.E., I.R., and Y.I. All authors have read andagreed to the published version of the manuscript.
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ACS Omega 2023, 8, 7858−7867

ACS Omega

http://pubs.acs.org/journal/acsodf

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This research was funded by Academic Leadership Grant(ALG) Prof. Iman Rahayu, Universitas Padjadjaran, grant
number ID: 2203/UN6.3.1/PT.00/2022.
Notes

The authors declare no competing financial interest.

■

ACKNOWLEDGMENTS

Authors are grateful for the facilities from Universitas
Padjadjaran, Indonesia, by Academic Leadership Grant(ALG), Prof. Iman Rahayu (ID: 2203/UN6.3.1/PT.00/
2022), Indonesian Ministry of Research by Penelitian Dasar
Unggulan Perguruan Tinggi (PDUPT ID: 2064/UN6.3.1/
PT.00/2022), and World Class Professor (WCP) 2022 grant.

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ArticleABBREVIATIONSDIC, Digital Image-based Colorimetry

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