Journal of Natural Fibers

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Ecofriendly Dyeing of Textiles with Natural Dyes

Extracted from Commercial Food Processing Waste
Materials

K. Amutha, S. Grace Annapoorani, P. Sakthivel & N. Sudhapriya

To cite this article: K. Amutha, S. Grace Annapoorani, P. Sakthivel & N. Sudhapriya (2022):
Ecofriendly Dyeing of Textiles with Natural Dyes Extracted from Commercial Food Processing
Waste Materials, Journal of Natural Fibers, DOI: 10.1080/15440478.2021.1993506

To link to this article: https://doi.org/10.1080/15440478.2021.1993506

Published online: 19 Feb 2022.

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JOURNAL OF NATURAL FIBERS
https://doi.org/10.1080/15440478.2021.1993506

Ecofriendly Dyeing of Textiles with Natural Dyes Extracted from

Commercial Food Processing Waste Materials
a
K. Amutha , S. Grace Annapoorania, P. Sakthivelb, and N. Sudhapriyac
a
Textiles and Apparel Design, Bharathiar University, Coimbatore, India; bDepartment of Nanoscience and Technology,
Bharathiar University, Coimbatore, India; cTextile Chemistry Division, The South India Textile Research Association,
Coimbatore, India

ABSTRACT KEYWORDS
Textile wet processing industry is one of the dreadful polluters in the world. Cotton; dyeing; natural dye;
An alternative to hazardous synthetic dyes could be dyes derived from nylon; spent coffee grounds;
various natural sources such as plants, insects, and minerals. Additionally, roasted peanut skin; silk;
agro-waste and food processing waste could serve as effective sources of circular economy
natural dyes. The current study focuses on extraction of natural dyes from 关键词
two commercial food processing waste materials, namely, the spent coffee 棉染色; 天然染料; 尼龙; 废
grounds and the roasted peanut skin. The dyes were found to possess rich 咖啡渣; 烤花生皮; 蚕丝; 循
tannin content and were applied on silk, cotton, and nylon fabrics with and 环经济
without the aid of mordants using water bath and ultrasonic bath. The dye
exhaustion percentage is better in water bath dyeing for spent coffee
grounds dye while its vice versa for the roasted peanut skin dye. Both the
dyes show good color fastness to washing with silk and nylon fabrics while
the grades are poor in case of cotton. However, the myrobalan and alum
mordanted cotton fabrics exhibit very good color fastness to laundering. The
color fastness to light is below average as is the case with most natural dyes.
The spent coffee grounds dye give yellow to light brown shades while the
roasted peanut skin dye give pink shades on cotton, silk, and nylon fabrics.
With the use of ferrous sulfate mordant the dyes give different shades of gray
color.
摘要
纺织湿加工业是世界上最严重的污染源之一. 从植物, 昆虫和矿物等各种自
然来源提取的染料可以替代有害的合成染料. 此外, 农业废物和食品加工废
物可作为天然染料的有效来源. 目前的研究重点是从两种商业食品加工废
料中提取天然染料, 即废咖啡渣和烤花生皮. 发现染料具有丰富的单宁含
量, 并使用水浴和超声波浴在有或无媒染剂的情况下应用于丝绸, 棉花和尼
龙织物上. 废咖啡渣染料水浴染色的上染率较高, 而烘烤花生皮染料水浴染
色的上染率较低. 这两种染料在丝绸和尼龙织物上均表现出良好的色牢度,
而在棉织品上则表现出较差的等级. 然而, myrobalan和明矾媒染棉织物具
有很好的耐洗色牢度. 与大多数天然染料一样, 耐光色牢度低于平均值. 废
咖啡渣染料在棉, 丝和尼龙织物上呈现黄色至浅棕色, 而烤花生皮染料呈现
粉色. 使用硫酸亚铁媒染剂后, 染料呈现出不同深浅的灰色.

Introduction
Natural dyes are generally derived from three major sources: plants, insects, and minerals.
Additionally, recent researches have explored natural dyes from agro-waste, food processing waste,
and unutilized or underutilized plant materials. Though natural dyes are ecofriendly natural dyeing
process could be noneco-friendly if heavy-metal-mordants like Chromium 6 (carcinogenic), Copper
sulfate (toxic, corrosive to skin and eye), Stannous chloride (cytotoxic and genotoxic), Zinc sulfate

CONTACT K. Amutha amuthatad@buc.edu.in Textiles and Apparel Design, Bharathiar University, Coimbatore, India
© 2022 Taylor & Francis
2 K. AMUTHA ET AL.

(aquatoxic), Zinc chloride (marine pollutant), etc. are used in the process. Natural mordants like
tannic acid, myrobalan (Terminalia chebula), Indian gooseberry (Phyllanthus emblica), pomegranate
rind, onion skin, etc. are used in place of metal mordants by researchers.
The waste released from food and beverage industry such as pressed berries and grapes, distillation
residues from strong liquor production, and wastes and peels from vegetable processing was used to
extract natural dyes for dyeing of woolen yarn (Bechtold et al. 2006). Pomegranate rind was used to
dye cotton fabrics with common salt (sodium chloride) as mordant that resulted in dyeing with good
fastness properties (Adeel et al. 2009). Natural dye from temple waste flowers (Tagetus erecta) was
used to dye cotton, silk, and wool fabrics along with various metal mordants Vankar (2009). Natural
dye from temple waste flowers (marigold) was used to dye soybean protein fabrics along with alum,
harda, tamarind seed coat, and amla as mordants (Teli, Sheikh, and Kamble 2013). Banana sap,
extracted from agro-waste, has been identified as an alternative to the Bridelia dye used by local
Adinkra cloth industry in Ghana (Dzomeku and Boateng 2013). Natural dyes extracted from the leaves
of guinea corn and onion skin were used to dye cotton fabrics with the addition of mordants such as
potassium dichromate, alum, iron sulfate and stannous chloride (Osabohien 2014). Natural dye
derived from coconut calyx (husk) was used to dye cotton fabrics with mordants such as pomegranate
rind, lemon rind, and alum that resulted in excellent wash and light fastness (Madhu, Rajni, and
Megha 2015).
Usually Nylon is dyed with acid and disperse dyes. Due to the negative impacts of these dyes on the
environment natural dyes may be used instead. Natural polyphenolic dyes were extracted from henna
leaves, pomegranate rind and Pterocarya fraxinifolia leaves to dye nylon 6 using aluminum sulfate,
tannic acid and tin chloride as mordants. The study suggests that tannic acid could be used successfully
as biomordant in place of metal mordants (Ebrahimi and Parvinzadeh Gashti 2016).
Freshly brewed coffee is preferred by consumers all over the world due to the stimulating effect,
strong and lingering aroma, and distinctive taste characterized by bitterness and sourness (Blumberg,
Frank, and Hofmann 2010). Chicory (Cichorium intybus) is a perennial plant with blue flowers; the
root of the plant is a long, fleshy tap root that yields a flavoring substance used as either additive or
substitute for coffee. Chicory perfectly mimics the bitter taste of coffee. Chicory is blended with coffee
as an economical choice because brewing of chicory-coffee blend consumes less compared to plain
coffee brewing. Worldwide, large amounts of coffee waste such as pulp, husk, and coffee beans are
generated daily. These residues contain substantial amounts of high value-added products for example
carbohydrates, proteins, pectins, and bioactive compounds as polyphenols, which could be extracted
and employed in the cosmetic, pharmaceutical, and food industries (Ramón-Gonçalves et al. 2019).
Espresso and cappuccino coffee are well-known beverages around the world, while in India ‘South
Indian filter coffee’ is renowned for its unique taste, aroma, and flavor. Either pure coffee grounds or a
blend of coffee and chicory in ratios like 95:5, 90:10, 85:15, 80:20, etc. are used to make South Indian
filter coffee. A special coffee filter made of metal, usually stainless steel, is used for brewing. Natural dye
was extracted from coffee, Coffea arabica, to dye cotton, silk, and wool fabrics with mordants such as
ferrous sulfate, copper sulfate, aluminum sulfate, manganous sulfate, stannous sulfate, and zinc sulfate.
The dyed samples exhibited average to good color fastness and good deodorizing property Lee (2007).
Natural dye has been extracted from Spent Coffee Grounds (SCGs) by a conventional solid–liquid
method to dye wool fabrics by infrared dyeing machine. The extract contains bioactive compounds
such as tannins, caffeine, and phenolic compounds. The dyed fabrics possess superior fastness proper­
ties with additional antioxidant ability and high levels of ultraviolet blocking (Koh and Hong 2019).
Peanut (Arachis hypogaea) is an annual legume crop of the pea family Fabaceae. The major peanut
producing countries in the world are India, China, Nigeria, Senegal, Sudan, Burma, and the United
States of America Madhusudhana (2013). India is the second-largest producer of peanuts next to
China with a total production volume of 6.7 million tons which accounts to 14% of the total world
production. Peanut skin, a by-product of the peanut processing industry, is rich in antioxidants like
phenolics but its economic value is regarded to be low. Three methods are adopted for skin removal:
direct peeling, blanching, and roasting. Roasting increases the phenolic content of the skin and the
 JOURNAL OF NATURAL FIBERS 3

total phenolics extracted with ethanol solvent is highest (Yu, Ahmedna, and Goktepe 2005). About 90–
125 mg total phenolics is present in a gram of dry peanut skin. Phenolic acids, flavonoids, and stilbene
are the main classes of phenolics present in peanut skin extracts. A study on the phenolic compounds
of the skin, hull, raw kernel, and roasted kernel flour of peanuts found that peanut skin contained
higher phenolic content and exhibited excellent antioxidant activity (Win et al. 2011).
Natural dye extracted from peanut red skin was used to dye wool with alum and ferrous sulfate
mordants. Dyeing was carried out by three methods: infrared, ultrasonic, and microwave. The dyed fabric
possesses good antibacterial activity against pathogens like Staphylococcus aureus, Klebsiella pneumonia
and a fungi, Candida albicans (Helmy et al. 2017). Roasted peanut skin was used to extract natural dye
and applied on cotton, silk, and wool fabrics by conventional and microwave dyeing. Apart from good
fastness properties the fabrics also exhibited ultraviolet protection, an UPF up to 65 (Ritu et al. 2018).
Both coffee beans and peanut skin are lighter in color in their raw state. Roasting process improves
their shade. Spent Coffee Grounds are rich in phytochemical components and nutrition but mostly they
are wasted. The roasted peanuts are de-skinned before human consumption because the skin tastes bitter.

Materials and methods

Materials
100% silk (20/22 Denier; Plain weave; EPI×PPI: 50×29; GSM: 50), 100% cotton (30 Ne; Single jersey
knit; WPI×CPI: 34×50; GSM: 145) and 100% nylon (80 Denier; Satin weave; EPI×PPI: 68×34; GSM:
75) ready-for-dye fabrics were used for the study.
The spent coffee grounds have been collected from a coffee shop in vicinity. This particular shop
uses a blend ratio of 95:5 coffee powder (Coffea arabica) and chicory (Cichorium intybus) to make
South Indian filter coffee. The residues of this blend after extracting decoction is found in paste like
consistency and hence dried under shade at room temperature and stored in airtight container until
further use. The waste skins were collected from a peanut sweet bar manufacturer in vicinity, ground
to powder using food processor and then used for dye extraction.
Myrobalan (Terminalia chebula) a common natural mordant and natural dye used in textile dyeing
has been chosen for the study. Two metal mordants that have comparatively least environmental
impacts, aluminum potassium sulfate (alum) and ferrous sulfate have also been used in dyeing.

Methods
Dye extraction
The powdered dye source materials were extracted with distilled water in water bath and ultrasonic
bath with a material to liquor ratio of 1:10 at 80°C for 1 h.

Mordanting of fabrics
In case of myrobalan, the powder is first boiled in water, MLR 1:10, for 1 h and cooled and filtered. The
fabric is treated with the filtrate for 1 h at boiling temperature by turning the fabric in the bath at
repeated intervals. In cases of alum and ferrous sulfate, the mordant is first dissolved in water (MLR
1:10), brought to boil and the fabric is treated for 1 h at boiling. The mordanted fabrics are squeezed,
dried under shade, and kept ready for dyeing.

Dyeing of fabrics
The control (unmordanted) fabric and the fabrics pre-mordanted with myrobalan, alum, and ferrous
sulfate were dyed at 80°C in water bath and ultrasonic bath for 1 h. After 1 h, the fabric is removed
from the dye bath, rinsed thoroughly in running water and dried under shade. The used dye bath still
contains colorants and hence the dye bath was reused for the second time to tie-and-dye silk fabrics.
The dyeing effluent was collected and refrigerated until analysis of effluent parameters.
4 K. AMUTHA ET AL.

Phytochemical analysis
The extracted dyes were analyzed for phytochemical composition, such as total phenol, tannin and
flavonoids. The phenolic compounds present in plants are good sources of natural dye. The total
phenolics of the dye extracts were determined by Folin-Ciocalteu method as described by Makkar
(2003). Gallic acid standard was also made and the results were expressed as Gallic Acid
Equivalents (GAE).
The amount of tannins was calculated by subtracting the nontannin phenolic from total phenolic as
mentioned by Makkar (2003), the analyses of total phenolic and free phenolic were also performed in
triplicates and the results were expressed in tannic acid equivalent (TAE).
The flavonoid contents of the extracts were quantified according to the method described by
(Zhishen, Mengcheng, and Jianming 1999). Rutin was used as standard and experiment was done in
triplicates and the results were expressed in Rutin Equivalents (RE).

FTIR spectroscopy
The Diffuse Reflectance Infrared Fourier Transform Spectra (DRIFTS) were obtained using a Jasco FT-
IR 4600 series with KBr pellet mode and a spectral window range of 4000–400 cm−1. Each KBr pellet
was made with 3 mg of dye extract and 100 mg of potassium bromide. In particular, freshly produced
KBr pellets were examined, with a total of 32 scans performed in a dry environment for each spectrum.

GC MS analysis
The dye extracts were analyzed using GC/MS (Agilent 7000 D GC/TQ) by DB 35-MS capillary
standard nonpolar column using Helium gas at a flow rate of 1.0 mL/min, initial temperature of
70°C increased to 260°C at the rate of 6°C to identify the compounds present. The dye was first
dissolved in methanol solvent at a concentration of 1 mg/ml and then analyzed using GC/MS by scan
mode and performed the library match to identify compounds.

UV-VIS spectroscopy
Jasco V-660 UV–Vis spectrophotometer is used for the current study. A sample of 100 microliter (µL)
is taken from the dye extract and transferred into 2 mL quartz cuvette and analyzed in the wavelength
ranging from 200 nm to 800 nm.

Color fastness testing

The color fastness of the dyed samples, to agents like laundering, rubbing, and light were determined
by standard test methods ISO 105 C06, ISO 105 X12 and ISO 105 B06, respectively.

Spectrophotometric analysis
Spectrophotometer is a versatile device used for the color measurement by reflectance or transmit­
tance or absorbance. The spectrophotometer designed specifically for color measurement of dyes and
dyed fabrics in dyeing industry operates under two modes: (1) transmittance (liquid samples) and (2)
reflectance (solid samples). Premier Colorscan spectrophotometer, Model SS 5100 H, with pulsed
Xenon light source with wavelength range from 360 nm to 700 nm is used for the study.
 JOURNAL OF NATURAL FIBERS 5

Reuse of dye bath

The dye bath is not completely exhausted even after one hour of dyeing. Hence an attempt has
been made to reuse the dye bath for the second time. Tie-and-dye method is a resist-dyeing
technique done manually to obtain colored patterns on fabric by gathering together small
portions of fabric and tying them tightly with string before immersing the cloth in the dye
bath. As the dye does not penetrate the tied portions of fabric, various patterns of coloring are
obtained on fabric which depends on the tying pattern. A notable advantage of tie-and-dye over
normal (plain) dyeing is that the uneven shade or patterns obtained in the former method makes
the possibility of reusing the dye bath. If normal dyeing is adopted while reusing the dye bath
the fabric may end up with patches, streaks, or uneven dyeing because some of the dyes have
already been exhausted from the dye bath and when premordanted fabrics are dyed some
unfixed mordant may get extracted in the dye bath. Hence, tie-and-dye is a suitable method
for reuse of dye bath.

Effluent analysis
The effluent has been analyzed for the 14 parameters prescribed by Pollution Control Board (PCB) by
standard or validated test methods at a Textile Research Lab accredited by ISO 17025.

Results and discussion

Phytochemical composition
Table 1 shows the phytochemical composition of the dye extracts. The spent coffee grounds dye is rich
in phenolics and tannins compared to the roasted peanut skin dye. The tannins in dye extracts would
serve as both dye and fixing agents. The flavonoid compounds impart color to the material. The dyes
extracted by ultrasonic bath possess better phytochemical composition than the water bath.

FTIR spectroscopy
The FTIR spectroscopy of the natural dyes extracted from the spent coffee grounds and roasted
peanut skin are shown in Figure 1a and b respectively. The broad peak at 3402 cm−1 (spent
coffee grounds dye) and 3420 cm−1 (roasted peanut skin dye) could be hydroxide (–OH) and
amine function groups stretching frequency corresponding to phenols, carboxylic acid in Gallic
acid-based tannins. The sharp peaks at 2919 cm−1 and 2926 cm−1 and weak peak at 2653 cm−1
may be C-H function group stretching frequency corresponding to aldehyde and allylic respec­
tively. The strong, sharp peak at 1626 cm−1 may be C = C function group stretching frequency
corresponding to unsaturated alkene and aromatic ring system. The medium and weak peaks at
1383 cm−1 and 1314 cm−1 may be – CH3 function group bending frequency and then 1132 cm−1
and 1119 cm−1 (Figure 1a and b) may be C–OH function group stretching frequency corre­
sponding to phenols, carboxylic acid in Gallic acid-based tannins.

Table 1. Phytochemical composition of dye extracts.

Extraction
Dye method Total phenol – GAE (mg/100 g) Tannin – TAE (mg/100 g) Flavonoid – RE (mg/100 g)
Spent coffee Water bath 33.78 ± 0.02 31.85 ± 0.19 10.32 ± 0.24
grounds Ultrasonic 37.12 ± 0.76 34.72 ± 0.72 10.37 ± 0.04
Roasted peanut skin Water bath 21.02 ± 0.05 19.47 ± 0.02 12.73 ± 0.35
Ultrasonic 24.88 ± 0.01 23.36 ± 0.01 13.95 ± 0.14
6 K. AMUTHA ET AL.

Figure 1. FTIR spectroscopy of dyes extracted from (a) spent coffee grounds and (b) roasted peanut skin.

GC MS
The presence of color compounds in spent coffee grounds and roasted peanut skin were illustrated in
the previous literature reports (Ana et al. 2012; Bae and Hong 2019; Elsorady and Ali 2018; Koh and
Hong 2019; Ritu et al. 2018). Based on the literature reports GC MS analysis was performed with
library match for the extracted dyes.
The compounds present in the dyes and their chemical structure are shown in Tables 2 and
3. The active sites in the color compounds that react with the mordant and fiber molecule are
shown in the chemical structure. The GC-MS spectra of the color compounds present in spent
coffee grounds dye and roasted peanut skin dye extracts with library match are shown in
Figures 2a, b and 3a, b, respectively. Melanoidins are dark brown natural coloring agents which
are responsible for the color of coffee extract and they can absorb light at 420 nm. Coffee

Table 2. Chemical structure of the dye compounds present in spent coffee grounds dye.
Category based on the
Common chemical nature and
Chemical name name functional group Chemical structure
Benz[c]coumarin-3-carboxylic acid, Coumaric Oxyaromatic acids
1,2,7- trimethoxy-, methyl(ester) acid
derivative

5,6,4 -trihydroxy Flavone Flavonoids

-7,8-dimethoxyflavone

! Reactive sites.
 JOURNAL OF NATURAL FIBERS 7

Table 2(B). Chemical structure of the dye compounds present in roasted peanut skin dye.

Category based
on the chemical
Common nature and
Chemical name name functional group Chemical structure
4-chloro-1,3,6- Arthothelin Xanthone
trihydroxy-8-methyl-
9 H-Xanthen-9-one

5,6,4 -Trihydroxy- Flavone Flavanoids

7,8-dimethoxyflavone

! Reactive sites.

melanoidins are composed of different chemical species such as Galactomannans,

Arabinogalactans, proteins, chlorogenic acids, and Maillard reaction products. Mordants assist
binding of dyes to fabric by forming chemical bridge from dye to fiber thus improving the
fixation of a dye along with increasing its fastness properties. 5,6,4ʹ-trihydroxy-7,8-dimethoxy­
flavone, a color component, Al3+ and cellulose were taken as an example to outline the reaction
mechanism. Initially, the metal ion Al3+ present in alum will make a co-ordination complex
with cellulose. Then it will react with 5,6,4ʹ-trihydroxy-7,8-dimethoxyflavone to form the co-
ordination complex using the aromatic alcohol and keto group as reactive site as shown in
Figure 4. The fibers made of proteins, such as silk, will make hydrogen bonding between the
polypeptide linkages and the dye.

UV-VIS spectra
The UV-VIS spectra of spent coffee grounds dye extracted by water bath (WCF1) and ultrasonic bath
(UCF1) are shown in Figure 5a. The ultrasonic extract showed two peaks at 279 nm and 326 nm while
the water bath extract at 280 nm and 324 nm. The UV-Vis spectra of the samples collected from the
dye bath (silk dyeing) after 30 min and 60 min of dyeing were analyzed and the same have been
presented in Figure 5b and c.

Table 3. Dye exhaustion percentage (E %).

Spent coffee grounds dye Roasted peanut skin dye
Time Ultrasonic dyeing Water bath dyeing Ultrasonic dyeing Water bath dyeing
30 min 2.01% 11.26% 82.68% 9.27%
60 min 3.02% 3.16% 91.67% 47.87%
8 K. AMUTHA ET AL.

Figure 2. GC-MS spectra of color compounds in spent coffee grounds dye extract with library match (a) Benz[c]coumarin-3-carboxylic
acid, 1,2,7-trimethoxy-, methyl(ester) and (b) 5,6,4ʹ-Trihydroxy-7,8-dimethoxyflavone.

The UV-VIS spectra of roasted peanut skin dye extracted by water bath (WGN1) and ultrasonic
bath (UGN1) are shown in Figure 6a. The ultrasonic extract showed two peaks at 259 nm and 364 nm
while the water bath extract at 282 nm and 314 nm. The UV-Vis spectra of the samples collected from
the dye bath (silk dyeing) after 30 min and 60 min of dyeing were analyzed and the same have been
presented in Figure 6b and c.
From the absorbance values, the dye exhaustion percentage after 30 and 60 min of dyeing are
calculated and tabulated in Table 4. The dye or extraction filtrate compound exhaustion percentage (%
E) was calculated by following empirical formula 1 (Vankar, Shanker, and Wijayapala 2011):

%E ¼½ðA0 Ar Þ=A0 �x100 (1)

where A0 and Ar are the absorbance of the dye bath before and after dyeing respectively at 326 nm λmax
of spent coffee grounds dye and 364 nm λmax of roasted peanut skin dye.
The dye exhaustion is better in ultrasonic dyeing than water bath dyeing, especially with roasted
peanut skin dye the difference is much higher (Table 4). Moreover ultrasonic dyeing is much energy
efficient than water bath (for 1 h of dyeing the energy consumption is 150 W using ultrasonic bath
while it is 3000 W using water bath).
 JOURNAL OF NATURAL FIBERS 9

Figure 3. GC-MS spectra of color compounds in roasted peanut skin dye extract with library match (a) 9 H-Xanthen-9-one, 4-chloro-
1,3,6-trihydroxy-8-methyl- and (b) 5,6,4ʹ-Trihydroxy-7,8-dimethoxyflavone.

Color fastness to washing (ISO 105 C06)

The color fastness of the dyed samples to washing/laundering have been analyzed and the grades are
assigned using ISO gray scales for color change and color staining (Table 5). The multifibre adjacent
fabric contains fabric strips such as acetate, cotton, nylon, polyester, acrylic, and wool.
With silk and nylon fabrics dyed with spent coffee grounds, the control (unmordanted) and
myrobalan, alum mordanted samples exhibited good color change grades ranging from 3/4 to 4/5; in
some samples darkening of the shade took place after laundering with soap as explained by (Trotman
1970). According to him, the vat dyes are always finished with a thorough soaping to remove the loose
pigments on the surface of the fabrics; however, the soap treatment has an effect on the shade. The
ferrous sulfate mordanted sample showed average to poor color fastness rating ranging from 2 to 4. Silk is
a protein fiber and always have good affinity toward natural dyes as like wool. Nylon is a polyamide fiber
and hence exhibit good fastness properties with the natural dyes. The cotton fabrics dyed with spent
coffee grounds, the control and myrobalan mordanted samples exhibited very poor color change grade of
10 K. AMUTHA ET AL.

Figure 4. Interaction between the color compounds, mordant, and fabric.

Figure 5. UV-VIS spectra of spent coffee grounds dye. (a) Comparison of UV-VIS spectra dyes by water bath (WCF1) and ultrasonic
bath extraction (UCF1). (b) UV-VIS spectra of ultrasonic bath dye extract, after 30 min of dyeing (UCF2) and 60 min of dyeing (UCF3)
(c) UV-VIS spectra of water bath dye extract, after 30 min of dyeing (WCF1) and 60 min of dyeing (WCF2).

Figure 6. UV-VIS spectra of roasted peanut skin dye. (a) Comparison of UV-VIS spectra of dyes water bath (WGN1) and ultrasonic bath
extraction (WGN2). (b) UV-VIS spectra of ultrasonic bath dye extract, after 30 min of dyeing (UGN2) and 60 min of dyeing (UGN3). (c)
UV-VIS spectra of water bath dye extract, after 30 min of dyeing (WGN2) and 60 min of dyeing (WGN3).
 JOURNAL OF NATURAL FIBERS 11

Table 4. Color fastness to washing (ISO 105 C06).

Dye Spent coffee grounds dye Roasted peanut skin dye

Mordant C M A FS C M A FS

Dyeing method W U W U W U W U W U W U W U W U
Color change Silk 4 4 4* 4* 3/4 4 3/4 3/4 4* 4* 4* 4* 3/4* 3/4* 2* 2*
Cotton 1/2 1/2 1/2 1/2 1 1 2/3 2/3 2/3 2 4 4 4/5 4/5 3/4 4
Nylon 4/5 4/5 4* 4* 4 4 4 4 4 4/5 3/4 3/4 4 4/5 3 3
Color staining on multifibre fabric 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5 4/5
Mordant: C: Control, M: Myrobalan, A: Alum, FS: Ferrous sulfate; Dyeing method: W: Water bath, U: Ultrasonic bath.
*Shade gets darker after soaping.

Table 5. Color fastness to rubbing (ISO 105 X12).

Dye Spent coffee grounds dye Roasted peanut skin dye

Mordant C M A FS C M A FS

Dyeing method W U W U W U W U W U W U W U W U
Silk, cotton, nylon fabrics Dry rub 5 5 5 5 5 5 4/5 4/5 5 5 5 5 5 5 4/5 4/5
Wet rub 4/5 4/5 4/5 4/5 4/5 4/5 3/4 3/4 4/5 4/5 4/5 4/5 4/5 4/5 3/4 3/4
Mordant: C: Control, M: Myrobalan, A: Alum, FS: Ferrous sulfate; Dyeing method: W: Water bath, U: Ultrasonic bath.

1/2; alum mordanted samples exhibited grade 1 while the ferrous sulfate mordanted samples showed
poor color fastness grade of 2/3. Natural dyeing of cotton is quite challenging, especially with natural
mordants. Cotton exhibits better fastness with heavy metal mordants like copper, tin, chromium, etc.
The roasted peanut skin dye exhibited excellent fastness on silk and nylon fabrics, control as well as
samples mordanted with myrobalan and alum, while cotton fabrics dyed well with myrobalan and alum
mordants only.

Color fastness to rubbing (ISO 105 X12)

Table 6 shows the color fastness to rubbing of silk, cotton, and nylon fabrics dyed with spent coffee
grounds and roasted peanut skin dyes with and without mordants. The control and myrobalan, alum
mordanted samples showed excellent rubbing fastness with dry rub rating of 5 and wet rub rating of 4/
5. Only in case of ferrous sulfate mordanted samples dry rub rating of 4/5 and wet rub rating of 3/4
have resulted.

Color fastness to light (ISO 105 B02)

Selected samples have been assessed for light fastness (Table 7). The fabrics dyed using dye extracted
by ultrasonic method have been selected. In cases of silk and nylon fabrics myrobalan mordanted and
in case of cotton alum mordanted samples were analyzed. The light fastness was found to be poor as is
the case with most natural dyes. The light fastness could be improved by suitable post treatments and
hence taken for further research.

Table 6. Color fastness to light.

Fabric Spent coffee grounds dye Roasted peanut skin dye
Silk 3 2
Cotton 2 2
Nylon 2 2
12 K. AMUTHA ET AL.

Table 7. Spectrophotometer values of fabrics dyed with spent coffee grounds dye.
K/S Spectrophotometer shades
Fabric Mordant Dyeing method L* a* b* C* h* ΔE λmax of dyed fabrics
Silk Control US 74.350 4.579 20.555 21.059 77.410 – 1.072

WB 76.624 3.644 18.019 18.384 78.536 3.532 0.780

Myrobalan US 76.085 1.313 23.748 23.784 86.800 – 3.720

WB 74.201 2.644 24.589 24.731 83.829 1.143 3.956

Alum US 74.550 3.591 21.978 22.269 80.688 – 1.172

WB 71.617 4.358 22.612 23.028 79.059 3.097 1.562

Ferrous sulfate US 60.792 4.355 21.054 21.500 78.282 – 2.940

WB 57.117 2.471 16.243 16.430 81.317 6.340 3.036

Cotton Control US 79.993 3.038 12.533 12.896 76.344 – 0.555

WB 82.778 2.411 7.739 8.106 72.667 5.580 0.331

Myrobalan US 73.945 2.887 16.957 17.191 80.300 – 1.118

WB 72.321 4.517 22.354 22.806 78.545 5.876 1.564

Alum US 76.889 2.897 13.068 13.385 77.469 – 0.719

WB 78.787 2.907 15.646 15.914 79.443 3.201 0.742

Ferrous sulfate US 71.122 2.833 12.063 12.391 76.753 – 1.023

WB 71.902 3.509 13.495 13.944 75.394 1.765 0.99

Nylon Control US 78.905 3.292 17.460 17.768 79.291 – 0.667

WB 79.335 3.066 16.639 16.919 79.527 0.954 0.617

Myrobalan US 68.656 3.331 26.778 26.984 82.876 – 3.517

WB 72.233 2.230 25.375 25.473 84.943 3.997 2.769

Alum US 78.192 3.248 17.048 17.355 79.181 – 0.704

WB 78.367 3.862 18.746 19.140 78.327 1.814 0.872

Ferrous sulfate US 71.927 4.770 19.436 20.013 76.180 – 1.219

WB 71.613 7.006 23.990 24.992 73.691 5.083 1.561

 JOURNAL OF NATURAL FIBERS 13

Spectrophotometric analysis
All the dyed fabric samples have been measured using spectrophotometer with color matching
software (Tables 8 and 9). CIE (International Commission on Illumination), is an international body
involved in standards development on colorimetry and photometry states Bhattacharyya (2010). CIE
system describes color in terms of L*a* b* C* h*, where,
L* is a measure of the lightness/darkness of an object and ranges from 0 (black) to 100 (white).
a* is a measure of redness (positive a*) or greenness (negative a*)
b* is a measure of yellowness (positive b*) or blueness (negative b*)
C* is a measure of chroma (saturation) and represents distance from the neutral axis.
h* is a measure of hue and is represented as an angle ranging from 0º to 360º, where,
0º–90º are reds;
90º–180º are yellow, yellow-green and greens;
180º–270º are green, cyan/blue-greens and blues;
270º–360º are blues, purples, magentas and return to reds.
The h value equal to 360º is reported as 0º.
The relationship K/S stands as the base for most computer color matching calculations. The
Kubelka-Munk equations are presented in Equations (2) and (3)

Rλmax ¼ 1 þ K=S½ðK=SÞfðK=SÞþ2g� (2)

or inversely,

K=S ¼ ð1 Rλmax Þ2 =2Rλmax (3)

where,
K is the absorption coefficient
S is the scattering coefficient
Rλmax is the reflectance at the wavelength of maximum absorption; here, λmax = 700 nm.
The total color difference (ΔE) is calculated from the Equation 3 as follows:

ΔE ¼½ðΔLÞþðΔaÞþðΔbÞ�1=2 (4)

where, ΔL = Ls – Lr, Δa = as – ar, Δb = bs – br

s,r represent sample and reference specimen, respectively.
The higher L values (ranging from 68 to 82 for spent coffee grounds dye and 69 to 82 for roasted
peanut skin dye) of unmordanted, myrobalan and alum mordanted samples show that the colored
fabrics are lighter in color. The lower L values (ranging from 57 to 71 for spent coffee grounds dye and
49 to 64 for roasted peanut skin dye) of ferrous sulfate mordanted samples show that the colored
fabrics are darker in color. Positive values of b* by samples dyed without mordant, myrobalan, alum
and ferrous sulfate mordants indicate yellowness. The color strength (K/S) values are less in case of
unmordanted samples and higher for mordanted samples.

Dye bath reuse

Silk fabrics were tie-and-dyed with spent coffee grounds and roasted peanut skin dye effluents with
mordants such as myrobalan, alum and ferrous sulfate. The dyes exhibited good dyeing patterns
especially with ferrous sulfate mordant. Hence, the reuse of dye bath is successful thereby making the
process sustainable.
 14

Table 8. Spectrophotometer values of fabrics dyed with roasted peanut skin dye.
K/S Spectrophotometer shades
Fabric Mordant Dyeing method L* a* b* C* h* ΔE λmax of dyed fabrics
Silk Control US 73.573 9.918 17.169 19.828 59.962 – 0.761

WB 79.070 7.398 14.041 15.871 62.191 6.808 0.440

K. AMUTHA ET AL.

Myrobalan US 69.441 7.987 22.986 24.334 70.811 – 1.866

WB 71.963 3.248 26.148 26.249 82.886 6.230 2.819

Alum US 74.477 6.246 14.433 15.727 66.572 – 0.699

WB 78.809 4.514 13.706 14.430 71.742 4.722 0.522

Ferrous sulfate US 51.202 3.476 5.251 6.297 56.474 – 2.339

WB 49.595 4.041 7.234 8.286 60.757 2.614 2.905

Cotton Control US 77.351 9.371 15.214 17.868 58.346 – 0.642

WB 78.365 8.998 14.454 17.026 58.073 1.321 0.587

Myrobalan US 78.294 4.408 18.550 19.067 76.602 – 0.910

WB 78.478 3.738 16.022 16.452 76.837 2.622 0.788

Alum US 76.932 6.759 13.541 15.134 63.448 – 0.577

WB 77.241 6.881 12.738 14.478 61.598 0.869 0.534

Ferrous sulfate US 58.069 4.165 7.056 8.194 59.424 – 1.820

WB 64.015 4.813 12.212 13.126 68.462 2.335 1.667

(Continued)
Table 8. (Continued).
K/S Spectrophotometer shades
Fabric Mordant Dyeing method L* a* b* C* h* ΔE λmax of dyed fabrics
Nylon Control US 80.600 6.305 10.063 11.875 57.907 – 0.315

WB 82.576 5.775 8.832 10.552 56.798 2.388 0.247

Myrobalan US 69.130 4.650 26.406 26.812 79.981 – 3.040

WB 68.806 4.237 25.664 26.011 80.593 0.909 3.150

Alum US 82.970 4.365 9.507 10.461 65.312 – 0.298

WB 82.939 4.299 9.100 10.064 64.687 0.413 0.280

Ferrous sulfate US 73.316 4.746 12.085 12.984 68.532 – 0.764

WB 75.275 3.850 10.247 10.946 69.380 2.857 0.705

JOURNAL OF NATURAL FIBERS
15
16 K. AMUTHA ET AL.

Table 9. Dyeing effluent parameters compared with synthetic dye and standard.
Result (untreated
effluent)
Spent
#
coffee Roasted * Standards for discharge of trade Characteristics of synthetic Standard
S. grounds peanut effluents (TNPCB B.P. Ms. No. 30 dye effluent (Yaseen and (for treated
no. Parameter dye skin dye Dated 21.02.1984) Scholz 2019) effluent)
1 pH at 30°C 4.6 6.78 5.5–9 5–10 5.5 to 9.0
2 Total dissolved 1600 1480 2100 50 2100
solids, mg/l
3 Total suspended 607 94 600 72–956 100
solids, mg/l
4 Color, Hazen 2430 7380 – 1450–4750 150 (PCU)
5 Turbidity, NTU 140 335 – – –
6 Chlorides as 490 175 1000 48–601 2.0
Cl-, mg/L
7 Sulfates as 510 560 1000 – –
(SO4)2-, mg/L
8 Sulfides as 0.16 0.13 2 – 2.0
S2-, mg/l
9 Phosphates as 62 30 5 – –
(PO4) 3-, mg/L
10 COD, mg/L 11000 4875 250 1100–4600 250
11 BOD (27°C, 3068 1614 350 10–1800 30
3 days), mg/L
12 Oil and grease, 40 18 20 – 10
mg/L
13 Phenolics, C6H5 4.48 42 5 – 1.0
OH, mg/L
14 % sodium 22.06 13.05 60 – –
*https://www.tnpcb.gov.in/pdf/tnpcb_you2013.pdf; #http://cpcb.nic.in/effluent-emission: Central Pollution Control Board, India.

Effluent analysis
The effluent means waste water left over by the end of dyeing process. Here, the effluent analyzed is
second effluent, means the extracted dye is first used to dye the fabrics and the dyebath is reused to tie-
and-dye silk fabrics. Finally, all the effluents collected are combined together and analyzed for fourteen
parameters (Table 10). Comparative values of the synthetic dye effluent, standards for discharge of trade
effluents (TNPCB), the standard norms for treated effluent as devised by the Central Pollution Control
Board, India have also been reported. Some parameters are found to be within the limits. The TDS and
TSS are within the permissible limits but the BOD and COD levels are higher since the dye is extracted
from natural materials, use of aqueous medium for extraction, the dyes rich in organic compounds, and
easy microbial growth. The higher color value in case of spent coffee grounds dye effluent need to be
studied further. A researcher (Lakshmi 2007) used 100% water, 50:50 water and natural dye effluent, and
100% effluent for irrigation of cow pea, horse gram and green gram seedlings at different stages of
growth and observed that 50:50 ratio water and natural dye effluent yielded better results in terms of
root and shoot growth. Hence natural dye effluent could be used for irrigation.

Table 10. Statistical analyses – Bonferroni test.

Dye exhaustion %
Spent coffee grounds dye Roasted peanut skin dye
Method 30 min 60 min 30 min 60 min
Ultrasonic 1 0.001 1 0.001
Water bath 1 0.129 1 0.001
 JOURNAL OF NATURAL FIBERS 17

Statistical analysis
Analysis of variance (ANOVA) is a statistical technique used to compare datasets. It is of three types: (i) one-
way analysis, (ii) two-way analysis, and (iii) K-way analysis. This method is most suitable for comparison of
two or more populations or samples. The most commonly used multiple comparison analysis statistics
include the following tests: Tukey, Newman-Keuls, Scheffee, Bonferroni, and Dunnett. Bonferroni adjust­
ment is a flexible post hoc method for making post hoc comparisons that ensure a family-wise type II error
rate no greater than α after all comparisons are made. The current study used one way ANOVA with
Bonferroni test using SPSS (Statistical Package for the Social Sciences) Statistics. The data have been tested
with ANOVA–Bonferroni test, Table 10, which shows that the difference is highly significant, with a p value
of 0.001 for ultrasonic method and 0.024 for water bath method, for dyeing up to 60 min than 30 min.

Conclusion
The current research shows that food processing waste such as spent coffee grounds and roasted peanut
skin could be effectively used in textile dyeing thereby transforming waste in to wealth as an approach to
circular economy. Such dyes reduce the effluent treatment load as they are biodegradable compared to
their synthetic counterparts. The solid waste residue obtained after dye extraction could be used in bio-
composting so as to retain circularity. The process promotes cleaner production and improves indus­
trial ecology. Further study may be required to improve the light fastness of these dyes. The study may
lead the future researchers to explore new dyestuff from other food processing waste materials.

Disclosure statement
No potential conflict of interest was reported by the author(s).

ORCID
K. Amutha http://orcid.org/0000-0002-2103-722X

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