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Harnessing natural colorants from algal species for fabric dyeing: a

sustainable eco-friendly approach for textile processing

Article in Journal of Applied Phycology · December 2019

DOI: 10.1007/s10811-019-01848-z

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Journal of Applied Phycology
https://doi.org/10.1007/s10811-019-01848-z

Harnessing natural colorants from algal species for fabric dyeing:

a sustainable eco-friendly approach for textile processing
Muhammad Azeem 1 & Naeem Iqbal 1 & Riffat Ayesha Mir 1 & Shahid Adeel 2 & Fatima Batool 1 & Ali Ahmad Khan 1 &
Sadaf Gul 3

Received: 12 March 2019 / Revised and accepted: 11 June 2019

# Springer Nature B.V. 2019

Abstract
Little information regarding the utilization of algal-based pigments in textile industry is available despite their abundance in
aquatic ecosystems, varying color nature, and relatively fast-growing habit than other photosynthetic organisms. The aim of the
current study is to optimize the conditions in order to harness the colorants from selected marine algal species and evaluating their
dye yielding potential for fabric dyeing. Cotton fabrics were dyed with aqueous, alkaline, acidic or organic extracts of four algal
species, the brown algae Iyengaria stellata, Sargassum muticum, Colpomenia sinuosa, and the red alga Laurencia obtusa under
varying conditions of temperature, pH, and exhausting agent concentration. Results showed that 4% KOH and 80% acetone
extraction produced maximum color strength of dyed cotton fabric. Among the four species of algae used in the study, L. obtusa
showed the highest yield of colorant. However, all four species extract behaved differently to dyeing conditions. Mordanting
experiments results revealed that iron sulphate and tannic acid were excellent pre- and post-mordanting agents for producing
darker color shades of cotton fabrics dyed with all the four algal species used in the study. FTIR analysis indicated that the
dominant coloring agents in all four algal species were phenolics in nature. The fabric dyed with extract of I. stellata, C. sinuosa,
and L. obtusa showed creamy white shade, while S. muticum-treated fabric produced light brown shade. Pre- and post-
mordanting of algal powder dyed fabric with chemical mordants, particularly the tannic acid produced other shades, such as
light and dark brown.

Keywords Color fastness . Cotton fabrics . Marine algae . Mordants . Natural dye

Introduction natural dye-yielding plants for extraction of colorant has

Widespread application of synthetic chemicals in textile pro-
cessing has led to serious environmental and human health
problems (Miah et al., 2017). An all-out use of sustainable
and ecofriendly synthetic chemicals in this area is still very
limited on account of limited availability and fewer color
shades (Bhuyan et al. 2004). The overutilization of few known
Electronic supplementary material The online version of this article
(https://doi.org/10.1007/s10811-019-01848-z) contains supplementary
material, which is available to authorized users.
* Naeem Iqbal
drnaeem@gcuf.edu.pk; naeemgc@yahoo.com
1
Department of Botany, Government College University Faisalabad,
Faisalabad, Pakistan
2
Department of Applied Chemistry, Government College University
Faisalabad, Faisalabad, Pakistan
3
Department of Botany, University of Karachi, Karachi, Pakistan
threatened the existence of these species and hence ecosystem
sustainability (Haji 2017: Adeel et al. 2018). Hence, there is a
dire need to search the abundantly available sources of natural
dyes that may not disturb the biodiversity and ecosystem bal-
ance (Yusuf et al. 2011; Raza et al. 2018). Considering the
rapid growth rate, variety of color shades, and widespread
occurrence of algae in different parts of the world, these may
be the best sources of natural dyes (Yusuf et al. 2011: Batool
et al. 2019: Mir et al. 2019) for industrial applications.
Algae, the dominant photosynthetic organisms distributed
both in fresh and marine water environments, are great source
of different photosynthetic pigments such as chlorophylls, ca-
rotenoids, phycobilins, phycocyanin, and phycoerythrin
(Shokry et al. 2010). Different algal groups are classified on
the basis of predominant pigments, such as chlorophyll b in
green algae (El-Khatib et al. 2016), fucoxanthin, and caroten-
oids in brown algae (Miyashita 2009; Peng et al. 2011) and β-
carotene and zeaxanthin in red algae (Schubert et al. 2006).
The pigments and dyes obtained from algae are used in a
number of applications, such as cosmetics, pharmaceuticals,

paints, and in paper industry (Ariede et al. 2017). Utilization of
algal pigments in the textile sector is negligible due to meager
availability of reports (El-Khatib et al. 2016) regarding the ex-
ploration of algal-based colorants in textile processing and lack
of information about extraction of dyes from algal sources.
Acetone extraction is generally considered the most effec-
tive and ecofriendly approach for efficient extraction of natu-
ral dyes (Michalak et al., 2015; Miah et al. 2016). Various
plant species, extraction techniques, and media have been uti-
lized to obtain the natural dye from photosynthetic organisms.
The extraction techniques include the heating, radiation, son-
ication (Manimozhi and Kanakarajan 2017), enzymatic ex-
traction (Billakanti et al. 2013), solvent extraction, and
super-critical fluid extraction (Miah et al. 2016). Similarly,
many extraction media have been reported for efficient extrac-
tion of natural colorant from different parts of photosynthetic
organisms. Algae, being the aquatic inhabitant, contain pig-
ments that are not usually soluble in water hence aquatic ex-
traction may not be a good strategy for obtaining dye from
algae. There is a great need to explore the species-specific
effective media for efficient extraction of natural colorant for
textile dyeing from algae.
The present study aims to provide a natural alternative of
synthetic chemicals for textile processing, by utilization of
abundantly available species of algae in the area. The objec-
tive of the study is to explore the relative dye-yielding poten-
tial of selected algal species and to find out the best condition
for colorant extraction from these species to be utilized in
textile industry.
Material and methods
Algal collection
Four algal species collected from marine habitats were tested
for their natural colorant potential during the present study.
The algal species, Iyengaria stellata (Børgesen) Børgesen
(Phaeophyceae), Sargassum muticum (Yendo) Fensholt
(Phaeophyceae), Colpomenia sinuosa (Mertens ex Roth)
Derbès and Solier (Phaeophyceae), and Laurencia obtusa
(Hudson) J.V. Lamouroux (Rhodophyceae) were collected
from coastal belt along Karachi, Pakistan. Colpomenia
simuosa was collected from intertidal zone of the coast of
Karachi (April 2014), while I. stellata was collected from
mid-littoral zone from Karachi coast (March 2014).
L. obtusa was collected from shallow rocky pools on lower
littoral zone (February 2014). Algal samples were washed,
oven dried at 70 °C for 3 days and ground to fine powder.
This powder was used for extraction of natural dyes. The
experiments were carried out at the Economic Botany Lab
of Department of Botany, Government College University,
Faisalabad.
J Appl Phycol
Colorant extraction
The colorant extraction was with various media. Aqueous,
alkaline (NaOH, KOH, Na2CO3), organic (ethanol and meth-
anol, acetone, N-hexane), ethanolic KOH, methanolic KOH,
and acidic media were used for colorant extraction.
Conventional method of aqueous extraction was employed
by mixing 3.0 g algal powder from each species used in the
study separately in 100 mL water. The aqueous extract was
prepared in water bath at 60 °C for 60 min. In case of colorant
extraction using different organic media (ethanol, methanol,
acetone, N-hexane), the dye extract of 3.0 g of dye powder
was prepared in various concentrations of each of solvent (20,
40, 60, or 80%) for 60 min at 60 °C. Three different alkaline
media (NaOH, Na2CO3, and KOH) were used to extract the
natural dye. Different concentrations of abovementioned alkali
(2, 4, 6, 8, or 10%) were treated with 3.0 g of dye powder of
each of algal species at 60 °C for 60 min in water bath. In case
of preparation of 2% ethanolic or methanolic KOH extraction
medium, 2.0 g KOH and 3.0 g of dye powder were added in
100 mL of ethanol or methanol and placed in water bath at
60 °C for 60 min. Acidic extraction medium was prepared by
using two levels of acid (1 or 2%) and 3.0 g of dye powder in
100 mL of media at 60 °C for 60 min in a water bath.
Optimization of dyeing parameters
The obtained extracts from abovementioned media were fil-
tered and labeled separately. The prepared natural dye extract
was used for dyeing cotton fabric. Dyeing conditions optimi-
zations were carried out using varying levels of dyeing vari-
ables. The exhausting agent (NaCl salt) was applied in differ-
ent concentrations such as 2, 4, 6, 8, or 10%. The dyeing
cotton fabrics were carried out at different pH levels (3, 5, 7,
9, or 11) of extraction media to find out optimum pH for each
algal species extract. To determine the optimum temperature
for each algal species extract, the dyeing process was carried
out at water bath temperature of 30, 45, 60, 75, or 90 °C. The
cotton fabrics dyeing were carried out separately for 15, 30,
45, 60, or 75 min. Color strength and lab values were evalu-
ated with the help of a Spectraflash SF 600 (Datacolor, USA)
spectrophotometer.
Results and discussion
Morphological characterization
The thallus of the C. sinuosa was greenish dark brown, ball
like, hollow, irregular, globular, lobed, surface smooth, at-
tached with substratum by disc holdfast. 6–70 cm in diameter.
Iyengaria stellata thallus was olive green in color, globular,
solid, thallus hollow from basal side, surface smooth with
J Appl Phycol
distantly arranged protuberances (stellata), margins entire; at-
tached with substratum by small rhizoidal disc, 5–12 mm
long. The thallus of L. obtusa was erect, cartilaginous, dark
red, 8–15 cm high, cylindrical, uniform diameter throughout,
base tapering, hold fast discoid, branches alternate, rarely op-
posite, ramuli short with obtuse or apices, bearing more
processes.
Color extraction
The results from color extraction experiments indicated that
all four algal species powder used in the study responded
differently to varying levels of extraction media (Table 1). In
general, basic media proved to be better used for extraction of
natural dye from algal species as compared with organic or
acidic ones. The colorant obtained from S. muticum produced
higher color strength (K/S) value on cotton fabrics when ex-
tracted in 4% NaOH solution. Almost similar K/S value was
recorded in cotton fabrics dyed with abovementioned algal
species based colorant extracted in 40% ethanol. The cotton
fabrics dyed with I. stellata powder showed relatively lower
color strength values in almost all extraction media compared
with the other three algal species used in the study. In this case,
8% methanolic KOH and 2% HCl proved better in getting
higher color strength than all other extraction media used in
this study. Colpomenia sinuosa powder yielded higher color
strength in 2% KOH and 1% HCl solution compared with
other extraction media. The natural colorants extracted from
L. obtusa powder produced higher color strength in 4% KOH
and 80% acetone as compared with other extraction media.
According to higher yield of colorant for textile dyeing, the
four algal species used in the study could be represented as
L. obtusa > S. muticum > C. sinuosa > I. stellata.
The greater solubility of algal-based colorants in basic
media indicated the compatibility of dyes towards OH-rich
environment to rapture the cell wall and maximum color-
ant extraction. The maximum solubility of S. muticum-
and L. obtusa-based dyes in 4% of NaOH and
C. sinuosa-based colorant in 2% KOH (Table 1) also in-
dicated their cost effectiveness. Similarly, 2% of HCl for
greater colorant extraction from I. stellata and 1% HCl
from C. sinuosa was economically good and gave higher
color depth of dyed cotton by rapid breakdown of cell
wall. However, excess of acid deteriorated the dye mole-
cules along with cell wall and degraded the cotton fabrics
(Shabbir, et al. 2016). Organic media proved to be effi-
cient in extracting maximum colorant within short time
and quickly hydrolyzed the cell wall of dye molecule
and gave maximum color strength onto dyed cotton fabric
(Huang et al. 2017). Overall, L. obtusa (red alga) gave
excellent outcome and produced higher level of color
strength (K/S value) using small concentration of alkali
as extraction media.
Optimization of dyeing parameters
The colorants extracted separately from the four algal
species used in the study produced higher color strength
of dyed cotton fabrics at varying conditions of dyeing
parameters optim a (Table 2). The ext ract from
S. muticum produced higher color strength values on
dyed cotton fabrics at 75 °C temperature and pH 9.0 of
the medium when dyed for 30 min time interval. Dyeing
of fabric with natural colorants for less than optimum
time might not be sufficient enough for complete ruptur-
ing of cell wall as well as moving of dye molecules
towards fabric (Ahmad et al. 2012). The less dyeing time
taken by algal powder, particularly obtained from
S. muticum and I. stellata to produce higher color depth
(Table 2) was not only economically efficient but also
helpful to maintain fabric strength.
The optimum of exhausting agent concentration (NaCl) for
this process was 4 g per100 mL dye solution. Cotton fabric
treated with extract of I. stellata showed higher color strength
value when dyed for 60 min at 75 °C keeping dyeing bath pH
at 9.0 using 4% NaCl as exhausting agent. It had been
established that color strength of dyed cotton fabrics was di-
rectly linked to salt concentration, used as exhausting agent
(Ahmad et al. 2012; Batool et al. 2013; Khan et al. 2014;
Hussaan, et al. 2017; Shahid et al. 2017). The results of pres-
ent experiments (Table 2) indicated that dye powder obtained
from S. muticum and I. stellata species required relatively less
salt (4%) to produce higher color strength compared with
other two algal species. Salt concentration below 4% was
not sufficient to form a firm bond between fabric and dye
molecule by neutralizing the negative charges. Salt concentra-
tion more than the optimal level in each case of all algal spe-
cies derived powder might had imbalanced the dye bath equi-
librium by forming precipitates and minimized the dye and
fabric interaction (Mondal and Razzaque 2007). The lower
exhausting agent requirements for algal-based natural colorant
to produce deeper shades indicated its ecological and econom-
ic significance.
The cotton fabrics treated with I. stellata extract pro-
duced higher color strength when dyed for 60 min.
Colpomenia sinuosa based natural colorant used for cotton
dyeing produced higher color strength (K/S) at pH 11
when dyed for 60 min at 60 °C keeping salt concentration
at 8%. Similarly, in case of cotton fabric treated with
L. obtusa extract, higher color strength values were ob-
tained at 30 °C dyeing temperature, 45 min dyeing time,
dyeing bath pH 7.0 and 6% salt concentration (Table 2).
Finding out the optimum temperature, a crucial step in
fabric dyeing with natural colorants had been the subject
of studies dealing with textile processing (Haji 2017;
Hussaan, et al. 2017; Adeel et al. 2018; Raza et al.
2018). Dyeing of fabric at temperatures other than
 J Appl Phycol

Table 1 Color strength values of

cotton fabrics dyed using natural Extraction medium Level % Sargassum Iyangaria Colpomenia Laurencia
dye extract from marine algal muticum stellata sinuosa obtusa
species using varying extraction
medium Aqueous 100 0.1673 0.0745 0.7698 0.2512
NaOH 2 0.1583 0.1203 0.5961 0.2576
4 1.1021 0.0743 0.134 0.227
6 0.8248 0.0802 0.2886 0.045
8 0.4235 0.0564 0.4056 0.0708
10 0.428 0.1262 0.3977 0.6477
KOH 2 0.4112 0.0652 1.0811 0.9645
4 0.5823 0.1148 0.7681 1.1677
6 0.4353 0.1248 0.8911 0.6462
8 0.6009 0.0733 0.9318 0.6787
10 0.3497 0.0578 0.7539 0.3212
Na2CO3 2 0.4109 0.0678 0.6902 0.4388
4 0.1919 0.0946 0.3482 0.7781
6 0.133 0.0459 0.9741 0.6933
8 0.1593 0.0292 0.8911 0.5151
10 0.5168 0.0488 0.8395 0.5672
Ethanol 40 1.0964 0.1467 0.5379 0.5371
60 0.0644 0.127 0.4591 0.4158
80 0.0736 0.1234 0.3014 0.73
Methanol 40 0.1796 0.1236 0.4902 0.4239
60 0.2828 0.2378 0.73 0.5545
80 0.2492 0.2282 0.4158 0.4422
Acetone 40 0.1763 0.1774 0.8487 0.2886
60 0.317 0.0678 0.8145 0.134
80 0.8487 0.0632 0.8699 1.1411
N-hexane 40 0.8145 0.0505 0.1796 0.5961
60 0.869 0.0393 0.2828 0.7698
80 0.745 0.0495 0.849 0.4881
Ethanolic KOH 2 0.0892 0.0574 0.3676 0.4318
4 0.2763 0.1688 0.1522 0.4422
6 0.2503 0.4283 0.1294 0.7681
8 0.152 0.055 0.1763 0.3977
10 0.1294 0.0643 0.317 0.4056
Methanolic KOH 2 0.4881 0.1407 0.4422 0.4902
4 0.3775 0.1082 0.3455 0.9741
6 0.3057 0.148 0.55455 0.6902
8 0.4282 0.679 0.4774 0.3482
10 0.3921 0.0798 0.4239 0.5399
Acidic medium (HCl) 1 0.8487 0.0287 0.9864 0.3507
2 0.8415 0.6351 0.4567 0.2763
3 0.7154 0.1522 0.5764 0.2503

optimum had been reported to produce poor color strength
of natural dyes (Shahid et al. 2017). Optimization experi-
ments results (Table 2) showed that all the four algal spe-
cies powder efficiently produced good color strength on
fabric at temperatures ranging from 30 to 75 °C. The pro-
duction of good color strength at 30 °C by L. obtusa
powder indicated its low energy requirements and eco-
nomic significance in dyeing process.
The relatively higher pH requirements of C. sinuosa
and S. muticum powder to produce good color strength
on cotton fabric indicated that greater number of OH
ions in dyeing bath favored rapid extraction of colorant
J Appl Phycol

Table 2 Effect of varying dyeing

parameters on the color strength Dyeing parameters Sargassum muticum Iyangaria stellata Colpomenia sinuosa Laurencia obtusa
values (K/S) of cotton fabrics
dyed by using dye extract of Time (min)
marine algal species 15 0.9874 0.3224 0.2263 0.2501
30 1.3795 0.6218 0.2286 0.3084
45 0.9433 0.4255 0.278 1.5269
60 0.771 0.6798 0.3262 0.3191
75 0.9366 0.8232 0.1754 0.3486
Temperature (°C)
30 0.9001 0.4214 0.2325 0.3745
45 0.9745 0.5661 0.2547 0.3568
60 0.9874 0.4418 0.7562 0.3276
75 1.9897 0.8632 0.3481 0.3187
90 1.0717 0.8456 0.3579 0.313
pH
3 0.9441 0.197 0.2454 0.2162
5 0.7054 0.6279 0.2856 0.3568
7 0.8703 0.427 0.2402 1.5269
9 1.3357 0.4922 0.2318 0.273
11 1.2929 0.4018 0.3423 0.3486
Salt concentration g(100 ml)-1
2 0.9506 0.3628 0.2476 0.2837
4 1.0325 0.6668 0.2509 0.3568
6 0.8803 0.3722 0.2527 0.6284
8 0.685 0.2801 0.2675 0.3281
10 0.9585 0.3486 0.25 0.3671

from these species. Overall, the algal species used in the that higher number of H ion (acidic pH of dyeing bath)
study had maximum dye yielding trend towards highly disturbed the dye bath equilibrium and repelled the algal
basic media except L. obtusa (Table 2). This indicated dye molecules resulting degradation of algal dye.

Fig. 1 Effect of Pre chemical mordants a CuSO4, b FeSO4, c TA, d Al2(SO4)3 on the color strength of cotton fabrics dyed using dye extract of marine
algal species

Fig. 2 Effect of Post chemical mordants a CuSO4, b FeSO4, c TA, d Al2(SO4)3 on the color strength of cotton fabrics dyed using dye extract of marine
algal species
Post and Premordanting
Treatment of cotton fabric with mordant chemicals before
dyeing using the extracts of the four algal species produced
varying shades with different color fastness and color strength
(Table S1, Figs. 1, 2). Pre-mordanting of S. muticum-treated
cotton fabrics with iron sulphate as well as tannic acid pro-
duced darker shades with 5 and 1% of concentration of men-
tioned mordants, respectively (Table S1; Fig. 1b, c). In case of
I. stellata treated cotton fabric, pre-mordanting with 7% tannic
acid produced higher color strength. Similarly, treatment of
cotton fabric with 7% tannic acid before coloring with
C. sinuosa extract produced darker shades with good color
strength values than those of all other mordant levels. Pre-
treatment of cotton fabric with 5% tannic acid produced
darker shades when dyed with L. obtusa extract.
Post-mordanting experiments results (Table S2; Fig. 2b)
showed that cotton fabric dyed with S. muticum extract pro-
duced darker shade when treated with 9% iron sulphate com-
pared with all levels of chemical mordants. Treatment of or
I. stellata extract dyed cotton fabrics with 9% tannic acid
produced darker shades with higher color strength values
among all mordants (Fig. 2c). Colpomenia sinuosa treated
cotton fabrics produced darker shades with 7% iron sulphate
compared with all other chemicals mordants used in the study.
Post-mordanting treatment of 3% tannic acid produced deeper
shades on L. obtusa-treated cotton fabrics than those of other
levels of mordants.
The results from mordanting experiments (Figs. 1 and 2)
indicated that the extract of all the four algal species used in
the study had potential to produce different color shades on
dyed cotton fabric upon treatment with chemical mordants.
J Appl Phycol
Overall, tannic acid and iron sulphate as pre- and post-
mordant significantly enhanced the color strength and pro-
duced darker shades to cotton fabric. The darker color shades
by mordanting with tannic acid indicated strong interactions
of this mordant with dye molecules to form insoluble complex
that firmly attached to cotton fabric (Ali, et al. 2010).
Similarly, iron constituted a firm bonding with dye molecules
as well as cotton fabric ultimately approaching towards max-
imum color strength onto algal-dyed cotton fabric (Bouatay
et al. 2016). Effectiveness of low concentrations metal salts,
tannic acid, and iron sulphate as pre- or post-mordants in
producing darker color shades indicated their cost-
effectiveness and environment friendly behavior.
The FTIR analysis
The FTIR analysis of L. obtusa dye extract revealed the pres-
ence of phenolics; the peak at 3362 cm −1 and 1200–
1550 cm−1 showed the presence of OH group and aromatic
ring, respectively (Fig. S1) that produced creamy white shade
of dyed cotton (Table 3). The FTIR analysis of S. muticum dye
extract resulted peaks at 3386 cm −1 as well as 1300–
1580 cm−1 indicating the presence of OH group and benzene
ring, respectively (Fig. S2). The FTIR results of C. sinuosa
dye extract revealed that OH group was present at the peak of
3373 cm−1 (Fig. S3) that resulted light brown shade of dyed
fabric (Table 3). While, bending peaks at 1300–1578 cm−1 as
well as 1619–1641 cm−1 represented the benzene ring and
CH 2 group, respectively. The FTIR analysis regarding
I. stellata-based dye extract indicated the presence of OH
group, CH2 as well as t aromatic ring at peak 3371 cm−1,
J Appl Phycol

Copper sulphate
1600–1678 cm−1, and 1439 cm−1, respectively (Fig. S4) thus

Grayish white
Grayish white
producing creamy white shade of dyed fabric (Table 3).
The FTIR analysis of dye extract of four algal species in-

White
White
dicated the functional group in dye extract responsible for
imparting color shades on cotton. The results revealed the
presence of phenolics substances in the dye powder of all algal

Aluminum sulphate
species used in the study that played crucial role in producing

Creamy white

Creamy white
Light brown
Light brown
different shades of dyed fabric. Phenolics have been demon-
strated in brown algae including S. muticum (Conde et al.
2015; Ayesha Mir et al. 2019) and red algae (Rengasamy
et al. 2015; Pangestuti et al. 2019).
Iron sulphate

Light brown
Light brown

Light brown
Light brown

Conclusion
Postmordanting

Sargassum muticum produced higher color strength on cotton

Dark brown
Dark brown
Dark brown
Tannic acid

fabrics at 75 °C temperature and basic pH of medium when

dyed for 30 min in the presence of 4.0 g per 100 mL NaCl as
Brown

exhausting agent. The cotton fabric dyed with I. stellata ex-

Color shade of dyed cotton fabrics using dye extracts of algal species without mordants and using varying mordants

tract at 75 °C, pH 5.0, using 4.0 g per 100 mL NaCl concen-

tration and 75-min time interval yielded higher color strength.
Copper sulphate

Grayish white
Grayish white

The optimum color strength by C. sinuosa was observed at

pH 11, dyeing for 60 min, 60 °C temperature, and 8.0 g per100
White

White

mL NaCl. The cotton fabric dyed by using L. obtusa dye

showed best trend towards color strength at 30 °C dyeing
temperature, 45 min time, pH 7.0, and 6.0 g per 100 mL
Aluminum sulphate

NaCl concentration.
Creamy white
Creamy white
Creamy white

Creamy white

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