Environmental Science and Pollution Research

https://doi.org/10.1007/s11356-018-1301-2

RESEARCH ARTICLE

Microwave-assisted extraction and dyeing of chemical

and bio-mordanted cotton fabric using harmal seeds as a source
of natural dye
Shahid Adeel 1 & Muhammad Zuber 2 & Fazal-ur-Rehman 2 & Khalid Mahmood Zia 2

Received: 30 November 2017 / Accepted: 15 January 2018

# Springer-Verlag GmbH Germany, part of Springer Nature 2018

Abstract
The revival of cultural heritage in a form of natural colorants for textile dyeing is gaining popularity due to their soothing nature
and bright shades. The present study was conducted to explore the coloring potential of harmala (Peganum harmala) seeds and to
improve color strength of dye using microwave radiations followed by a mordanting process. The results showed that harmala
plant seeds could be an excellent source of natural dyes for cotton dyeing if the irradiated acidified methanolic extract (RE, 4 min)
is used to dye un-irradiated fabric (NRC) at 85 °C for 45 min using a dye bath of pH 9.0 having salt concentration of 7 g/100 mL.
Alum (1%) as pre-mordants and iron (7%) as post-mordants have improved the color strength in chemical mordanting more than
other mordants employed. The bio-mordants employed reveal that 10% of acacia as pre-bio-mordants and 7% of acacia as post-
bio-mordants are effective amounts to obtain high color strength. Suggested ISO standards for colorfastness illustrate that bio-
mordanting has given more excellent rating as compared to chemical mordants. It is concluded that harmala seeds have a great
potential to act as a source of natural colorant for cotton dyeing under the influence of microwave radiation.

Keywords Cotton . Bio-mordanting . Colorfastness . Harmal . Microwave radiation . Spectraflash SF 600

Introduction (Vankar et al. 2011). Now, these associations such as

The revival of cultural heritage for decorating different aspects
of life such as clothes, cosmetics, paints, and varnishes is due to
ecofriendly nature of colorants derived from plants, animals, and
minerals (Guoco et al. 2011; Dayioglu et al. 2015). This resur-
gence is due to censuring the frequent use of synthetic dyed
products, because the effluent loads of synthetic dyes and other
associated chemicals involved during their preparation cast very
hazardous effects on the ecosystem and enhance global warming
Responsible editor: Philippe Garrigues
Electronic supplementary material The online version of this article
(https://doi.org/10.1007/s11356-018-1301-2) contains supplementary
material, which is available to authorized users.
* Shahid Adeel
shahidadeel@gcuf.edu.pk
1
Department of Chemistry, Govt. College University,
Faisalabad 38000, Pakistan
2
Department of Applied Chemistry, Govt. College University,
Faisalabad 38000, Pakistan
Environment Potential Agency (EPA), Food and Agriculture
Organization (FAO), Ecological and Toxicological
Associations of Dyes and Organic Manufacturers (ETAD),
and Global Organic Textile Standards (GOTS) have forced
the consumers, traders, and researchers to move towards
natural dye (Shukla and Vankar 2013). The wonderful ben-
efits of natural dyes are due to the nature’s blessings, their
Ayurvedic nature, and esthetic values as these dyes have
antimicrobial, antioxidant, antipyretic, anti-inflammation, an-
ti-hemolytic, antiviral, and other several properties (Kasiri
and Safapour 2014; Devi et al. 2017). These dyes are also
the part of our heritage because in the past, these dyes were
used to decorate the caves, walls, bodies (to attain some
magical power), fabric, etc. (Petroviciu et al. 2012).
A lot of plant-based natural colorants have been explored for
dyeing of cotton, wool, and silk fabrics (Haji 2013, 2017; Baaka
et al. 2017), but literature have no evidence for utilization of
harmal seeds (Peganum harmala) as a source of natural color-
ants. It is one of the oldest traditional plant commonly known as
wild rue that belongs to the Zygophyllaeceae family and is
found in Asia, Australia, and North America (Niroumand et al.
 Environ Sci Pollut Res

2015; Moradi et al. 2017). Seed is the important part of the plant
which is utilized in modern phytotherapy and old Ayurvedic
system. Several alkaloids such as (harmalacidine,
tetrahydroharmine) (Tascon et al. 2017), β-carboline, and
quinazoline derivatives (vasicine, vasicinone, deoxyvascicinone)
are the important phytochemicals (Herraiz et al. 2017). The col-
oring behavior of harmala seeds is due to the presence of alka-
loids (Dos Santos and Hallak 2017) called harmine, harmol,
harmaline, and harmalol (structures given below) that give
yellowish red color and is considered as an alternative to the
Turkey red that is obtained from madder (Wang et al. 2015).
This yellowish red dye has been used to dye wool and carpets.
Harmala seed is the source of a fluorescent natural dye that
exhibits hypothermic and hallucinogenic characteristics and is
used for making ink, tattoos, and rug and wool dyeing. It also
exhibits antipyretic, antidiuretic, antimicrobial, anti-parasitic, an-
ti-viral, anti-parasitic, anti-plasmodial, anti-depressent, and anti-
tumor activity characteristics and is used to cure remillent fever,
chronic malaria, anti-inflammatory, and headache (Reddy et al.
2017; Li et al. 2017; Mashhadi et al. 2016).

H3CO H H
N HO
CH3 N CH3

N N

Harmaline Harmalol

H H
N CH3 H3CO
N CH3

N N

Harmane Harmine

Due to these wonderful health benefits of harmala seeds,
the current study has been undertaken to explore its dyeing
behavior completely from extraction to mordanting under
the influence of microwave treatment. Nowadays, there is
an urge to use such colorants in textiles, cosmetics, fash-
ion, etc. due to their sustainability and reviving the cultural
heritage around the globe. For the improvement of the nat-
ural dyeing process, scientists are using many methods to
tune the fabric surface and to enhance the extraction yield
(Zahid et al. 2017). They are employing traditional as well
as modern methods including enzymes (Nguyen et al.
2017), gamma (Gulzar et al. 2015; Usman et al. 2016;
Adeel et al. 2017a, b), ultraviolet (Rehman et al. 2017;
Iqbal et al. 2008) plasma (Haji et al. 2014), and ultrasonic
treatment (Ticha et al. 2017). However, microwave is one
of the modern methods that have been used for the extrac-
tion and dyeing of natural fabrics with low consumption of
energy, time, and labor. These radiations increase the
movement of dye material to the solvent and enhance the
significant mass transfer effects (Karabegovic et al. 2012;
El-Khatib et al. 2016; Sivakumar et al. 2017). Previous
studies also show that microwave radiation (MW). not only
provides leveled heating to the substrate but also adds val-
ue in coloration of natural fabrics via a unique mechanism.
Keeping in view the benefits of microwave treatment and
its cost-effective benefits, the aim of the current study is to
explore the harmal seeds as possible source of yellowish
natural dye and to improve the color characteristics of
Environ Sci Pollut Res

Fig. 1 a Effect of different a

microwave radiation time on 4.5
powder of harmala seed. b Effect
of different microwave radiation 4
time on extracted dye. c Effect of
3.5
different microwave radiation
time on extraction 3
2.5 NRP/NRC

K/S
2 RP/RC
1.5 RP/NRC
1 NRP/RC

0.5
0
1 min 2 min 3 min 4 min 5 min 6 min
Radiation time (min)
b
12

10

8
NRE/NRC
K/S Value

6 RE/RC
RE/NRC
4
NRE/RC
2 Simultaneous
0
1min 2min 3min 4min 5min 6min
Radiation time (min)
c
2
1.8
1.6
1.4
1.2
K/S

1 NRS/NRC
0.8 RS/RC
0.6 RS/NRC
0.4
0.2
0
1min 2min 3min 4min 5min 6min
Radiation time (min)

chemical and bio-mordanted fabrics under the influence of
microwave radiation.
Materials and methods
Material collection
Harmal seeds (Peganum harmala L.) commonly known as
wild rue has been procured from Faisalabad, Pakistan, washed
with distilled water, and dried under shade. The powder of
uniform particle size was obtained by finely grinding the dried
seeds followed by passing through the sieve of 20 mesh.
Pretreated cotton fabrics were obtained from Noor Fatima
Fabrics, Faisalabad, Pakistan. All the chemicals used during
extraction such as methanol, conc. hydrochloric acid (HCl),
sodium hydroxide (NaOH), Glauber’s salt/sodium sulphate
(Na2SO4), table salt/sodium chloride (NaCl), and mordants
such as iron sulphate (FeSO4), copper sulphate (CuSO4),
Fig. 2 FTIR analysis of un-
irradiated (NRC) (a) and
irradiated (RC, 4 min) (b) cotton
fabric
Environ Sci Pollut Res
aluminum sulphate (Al2[SO4]3), tannic acid, tin chloride
(SnCl2), and cobalt chloride (CoCl2) were of commercial
grade (Pakistan made). For bio-mordanting, turmeric rhi-
zomes, henna leaves, acacia bark, and pomegranate rind were
purchased from the local market and were subjected to extract
the bio-mordants by following already documented methods
(Rather et al. 2017).
Extraction and irradiation process
For Microwave treatment (MW treatment), powder, extracts,
and fabrics were irradiated for 1–6 min at high power using a
commercially available orient oven of 50 Hz with the power
of 700 W. Four media such as aqueous, alkaline, acidic, and
organic (methanol) have been employed to extract the colorant
from irradiated (RP) and un-irradiated powder (NRP). For
comparative study, the extracts have also been irradiated up
to 6 min which have been employed to dye irradiated (RC)
and un-irradiated fabric (NRC). In another series of
Environ Sci Pollut Res

4.5
4
3.5
3
2.5

K/S
2
1.5
1
0.5
0
35 45 55 65 75 85
Temperature ( °C)

Fig. 5 Effect of different temperature on dyeing of un-irradiated cotton

(NRC)

Optimization of dyeing and mordanting conditions

Different dyeing parameters such as temperature, time, pH,

Fig. 3 SEM analysis of un-irradiated (NRC) (a) and irradiated (RC,
4 min) (b) cotton fabric
experiment, microwave-assisted extraction (MAE) has also
been carried to compare the K/S values with other adopted
methods. For extraction of dye before and after irradiation
treatment, an appropriate amount of powder has been
employed by boiling for 1 h in selected solvents keeping
material-to-liquor ratio of 1:25.
3 4.5
2.5
2 3
K/S
material-to-liquid ratio, and salt concentration were opti-
mized. Dyeing of un-irradiated fabric (NRC) was carried
out at 25, 30, 40, 55, 70, and 85 °C using optimal extract
for 25, 30, 40, 55, 70, and 85 min. In another set of exper-
iments, by varying the medium of a dye bath, extracts of
7,8, 9, 10,11, and 12 pH were employed using material to
liquid ratios of 1:25. To achieve maximum exhaustion, 1,
3, 5, 7, or 9 g/L of salts (Na2SO4 and NaCl) were added
during dyeing of un-irradiated fabric (NRC) using the acid-
ified methanolic extract. For improvement of color
strength (K/S) and color fastness properties, 1, 3, 5, 7, 9,
and 10% of chemical mordants such as Cu (Copper
Sulphate), Al (potash alum), Fe (iron sulphate), Sn (tin
chloride) Co (cobalt chloride), and TA (tannic acid) and
bio-mordants such as turmeric (curcumin), pomegranate
(tannin), henna (lawsone), and acacia ’s extracts
(quercetin) were employed as pre-mordanting and post-
mordanting at optimal conditions. For extraction of bio-
mordants from plant sources, the crude powders of respec-
tive plants were boiled with distilled water for 1 h keeping
material-to-liquor ratio of 1:25.
4
3.5
2.5
K/S

1.5
2
1 1.5
1
0.5
0.5
0 0
2 4 6 8 10 35 45 55 65 75 85
Powder (g) Time (min)

Fig. 4 Effect of different concentration of dye powder on dyeing of un- Fig. 6 Effect of different time on dyeing of un-irradiated cotton (NRC)
irradiated cotton (NRC)
 Environ Sci Pollut Res

2.5
irradiated for 5 min and extraction is carried out in a meth-
2 anolic medium, maximum color strength is obtained onto
un-irradiated fabric (Fig. 1a). Similarly, if the acidified
1.5 methanol extract is irradiated for 4 min (RE/NRC), then
K/S

it gives darker shade and high color strength onto un-

1 irradiated fabrics (Fig. 1b). In another series of experi-
0.5
0
1 2 3 4 5 6 7 8 9 10 11
pH
Fig. 7 Effect of different pH on dyeing of un-irradiated cotton (NRC)
Evaluation of characteristics of dyed and undyed
fabrics
For observing the influencing Microwave (MW treatment),
FTIR and SEM analysis of treated and un-treated fabrics were
carried out. For evaluation of color strength (K/S), all the dyed
fabrics were subjected to CIE Lab system computed in
spectraflash SF600 equipped with an illuminant of D 65 10°
observer at the Department of Applied Chemistry Government,
College University of Faisalabad, Pakistan. To observe the role
of bio-mordants in comparison with chemical mordants, the
dyed fabrics were subjected to ISO standards to rate the color
fastness properties. For the purpose, washing fastness was rated
using ISO 105 CO3 in rota wash, light fastness was rated using
ISO 105 BO2 in fadometer, and crocking (rubbing) was rated
using ISO 105 X-12 through crock meter.
ments, the simultaneous extraction (MAE) reveals that ir-
radiation for 3 min gives good color strength onto un-
irradiated fabric (Fig. 1c). This is because microwave ra-
diation causes mass transfer effect from substrate to sol-
vent, thereby rupturing the cell wall (Shang et al. 2016;
Franco-Vega et al. 2016). It also facilitates the solvents to
extract out the main colorant from substrate without caus-
ing any degradation in short time. Hence, by employing
different solvents, it is observed that the acidified methanol
has high dissipation power and high MW absorptivity and
polarizability due to which maximum color yield has been
obtained by employing the extract onto un-irradiated fabric
(Patil and Akamanchi 2017; Adeel et al. 2017a, b). Short
duration of irradiation does not evolve colorant well into
solvent, while irradiation for long time may involve other
impurities to evolve into solvent along with colorant,
which upon dyeing influences the coloration of fabric.
Hence, comparatively, if the extract is irradiated for
4 min (RE), the alkaloids present in harmal are stimulated
a
5
4.5
4
3.5
Copper
3
Tin
K/S

Results and discussion 2.5

Cobalt
2
Aluminium
1.5
The results displayed in Fig. 1a for irradiation of powder, Iron
1
Fig. 1b for irradiation of extract, and Fig. 1c for simulta- T.A
0.5
neous extraction, i.e., microwave-assisted extraction
0
(MAE), reveal that MW treatment to extract RE for 1 3 5 7 9 10
4 min has shown promising results onto un-irradiated fab- Mordant Concentration (%)
ric (NRC). It has been found that if harmal powder is b
3
3.5
Na2SO4 (%) 2.5
3 NaCl
2 Copper
2.5
Tin
K/S

2 1.5
Cobalt
K/S

1.5 1 Aluminium
Iron
1
0.5
T.A.
0.5
0
0 1 3 5 7 9 10
1 3 5 7 9 Mordant concentration (%)
Salt (%)
Fig. 9 Effects of different concentrations of pre-chemical mordanting (a)
Fig. 8 Effect of different salt concentration on dyeing of un-irradiated and post-chemical mordanting (b) on dyeing of un-irradiated cotton
cotton (NRC) (NRC)
Environ Sci Pollut Res

a and interact with the acidified methanol through mass

4.5
transfer kinetics and, upon dyeing of un-irradiated fabric
4
(NRC), give darker shade with high color strength.
3.5
The chemical changes of fabric have been revealed by
3
FTIR analysis (Fig. 2a, b). MW treatment did not change the
2.5 Acacia
chemical structure of the cellulose; however, it may change
K/S

2 Henna
the orientation of the region to interact with the colorant in a
1.5 Turmeric
plane more significantly. The morphological changes have
1 Pomegranate
been observed by SEM analysis (Fig. 3a, b). The images show
0.5
that there might be some changes occurred at the surface of the
0
1 3 5 7 9 10 fabric which, in turn, helps to make significant interaction
Mordant Concentraon (%) with the colorant. Hence, for getting maximum K/S, the irra-
b diated acidified extract (RE, 4 min) is optimized to dye un-
3.5
irradiated fabric (NRC).
3 The results given in Fig. 4 reveal that 8 g of powder used for
2.5 obtaining extract in the acidified methanol has been optimized
followed by irradiation for 4 min. This is because irradiation of
2 Acacia
extract using an optional amount gives maximum coloration onto
K/S

1.5 Henna
un-irradiated fabric via leveled heating. Too low amount did not
Turmeric
1 give high K/S due to extraction of low color yield, whereas too
Pomegranate
high amount of powder may give significant chance to involve
0.5
other phytochemicals along with colorant at greater extent during
0 coloration, thereby affecting the color strength. Hence, to achieve
1 3 5 7 9 10
Mordant concentration (%) maximum color yield, 8 g of powder is optimized. The reduction
Fig. 10 Effects of different concentrations of pre-bio-mordanting (a) and
in amount of powder reveals that MAE is a cost-effective process.
post-bio-mordanting (b) on dyeing of un-irradiated cotton (NRC) Optimal temperature in the natural dyeing process gives
high color strength because it helps to achieve the equilibrium

Table 1 Effect of pre-mordants on the color characteristics of un-irradiated cotton fabric (NRC) dyed at optimal conditions

Mordant conc. (%) Al Fe Sn Cu

LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF LF

Control 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4
1 3/4 4/5 4/5 4 4 4/5 4/5 4 3/4 4 4 4/5 4
3 3/4 4 4 3/4 4/5 4 4/5 4 4/5 4 4/5 4 4/5
5 4 4/5 4/5 4 4 4/5 4 3/4 4 4/5 4 4/5 4
7 4 4/5 4 4/5 4/5 4/5 4 4 4/5 4/5 4 4 4/5
9 4 4 4 4/5 4/5 4 4/5 3/4 4/5 4 4/5 4 4/5
10 4 4 4/5 4/5 4 4 4/5 3/4 4 4/5 4/5 4/5 4

Mordant conc. (%) Cu TA Co

WF DRF WRF LF WF DRF WRF LF WF DRF WRF

Control 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4

1 4 4 3/4 4/5 4 4 3/4 4 4/5 4 3/4
3 4/5 4 3/4 4 4/5 4 3/4 4/5 4/5 4/5 4
5 4 4/5 4 4/5 4 4/5 4 4 5 4 4/5
7 4 4 4 4/5 4/5 4 4 4/5 4/5 4/5 4
9 4/5 4/5 4/5 4/5 4/5 4 4 4/5 4/5 4 4/5
10 4 4/5 4/5 4/5 4 4/5 4/5 4/5 4/5 4/5 4/5

LF light fastness, WF wash fastness, DRF dry rubbing fastness, WRF wet rubbing fastness
 Environ Sci Pollut Res

Table 2 Effect of pre-bio-mordants, on the color characteristics of un-irradiated cotton fabric (NRC) dyed at optimal conditions

Mordant conc. (%) Turmeric Henna Acacia Pomegranate

LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF

Control 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4
1 3/4 4/5 4/5 4 4/5 4/5 4 3/4 4 4 4/5 4 4 4 3/4
3 3/4 4 4 3/4 4 4/5 4 4/5 4 4/5 4 4/5 4/5 4 3/4
5 4 4/5 4/5 4 4/5 4 3/4 4 4/5 4 4/5 4 4 4/5 4
7 4 4/5 4 4/5 4/5 4 4 4/5 4/5 4 4 4/5 4 4 4
9 4 4 4 4/5 4 4/5 3/4 4/5 4 4/5 4 4/5 4/5 4/5 4/5
10 4 4 4/5 4/5 4 4/5 3/4 4 4/5 4/5 4/5 4 4 4/5 4/5

LF light fastness, WF wash fastness, DRF dry rubbing fastness, WRF wet rubbing fastness

of the dye bath. Low heating does not enhance rate of striking,
whereas too much heating may cause desorption of dye com-
ponent from fabric resulting into low color strength (Shahid
et al. 2017). The results given in Fig. 5 show that 85 °C is the
optimal dyeing temperature.
Contact time in natural dyeing also plays a vital role be-
cause it is related with rate of diffusion of colorant with fabric.
Low contact time imparts low coloration due to low kinetic
energy of molecules, whereas high contact time may degrade
the colorant that favors the rate of stripping (Khan et al. 2012).
Hence, dyeing of un-irradiated fabric (NRC) for 45 min using
the irradiated acidified methanolic extract (RE, 4 min) gives
high color strength (Fig. 6). The medium of the dye bath is
very important because it helps in making covalent inter-
action of negatively charged surface of cellulosic fabrics
with colorant. Too much acidic medium did not add value
in dyeing of fabric due to addition of extra H+ ion, while
too much alkaline medium may swell the fabric and
weakens the fibers to hold the dye more promisingly. The
results given in Fig. 7 show that dyeing of un-irradiated
fabric (NRC) has given good color strength by employing
dye bathof pH 9. Exhausting agents in any dyeing process
plays good role for firm interaction because it creates the atmo-
sphere around water, colorant, and fabric to come within short

Table 3 Effect of post-modants, on the color characteristics of un-irradiated cotton fabric (NRC) dyed at optimal conditions

Mordant conc. (%) Al Fe Sn Cu

LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF LF

Control 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4
1 3/4 4/5 4/5 4 4/5 4/5 4/5 4 3/4 4 3/4 4/5 4
3 4 4/5 4 4/5 4/5 4 4/5 4 4/5 4/5 4/5 4 4/5
5 4/5 4/5 4/5 4 4 4 5 4/5 4 4/5 4/4 4/5 4
7 4/5 4/5 4/5 4/5 4/5 4/5 5 4 4/5 4 4 4 4/5
9 5 4 5 4/5 4/5 4/5 4/5 4 4/5 4/5 3/4 4 4/5
10 4/5 4/5 4/5 4/5 4 4/5 5 4/5 4 4 4 4/5 4

Mordant conc. (%) Cu TA Co

WF DRF WRF LF WF DRF WRF LF WF DRF WRF

Control 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4

1 4 4 3/4 4/5 4 4 3/4 4 4 4 3/4
3 4/5 4 4/5 4 4/5 4 4 4/5 4 4 4
5 4 4/5 4/5 4/5 4/5 4/5 4/5 4 4/5 4/5 4
7 4 4 4/5 4/5 4/5 4/5 4 4/5 4/5 4 4
9 4/5 4/5 4 4/5 4/5 5 4/5 4/5 4/5 4/5 4
10 4 4/5 4 4/5 4 5 4/5 4/5 4/5 4/5 4

LF light fastness, WF wash fastness, DRF dry rubbing fastness, WRF wet rubbing fastness
Environ Sci Pollut Res

Table 4 Effect of post-bio-mordants, on the color characteristics of un-irradiated cotton fabric (NRC) dyed at optimal conditions

Mordant conc. (%) Turmeric Henna Acacia Pomegranate

LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF LF WF DRF WRF

Control 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4 3/4 3/4 4 3/4
1 3/4 4/5 4/5 4 4 4/5 4 4 3/4 4 4 4 /54 4 4/5 4
3 3/4 4 4 3/4 4 4 4 4 4/5 4 4/5 4 4/5 4 4/5 4
5 4 4 4/5 4 4/5 4/5 4/5 3/4 4/5 4/5 4/5 4/5 4/5 4/5 5 4/5
7 4/5 4 4 4 5 4/5 4/5 4 5 4/5 4/5 4/5 5 4/5 4/5 4
9 5 4 4 4 5 4 5 4 5 4/5 5 4/5 5 5 4/5 4
10 5 4 4/5 4 5 4 5 4 4/5 5 5 4/5 4/5 5 4/5 4/5

LF light fastness, WF wash fastness, DRF dry rubbing fastness, WRF wet rubbing fastness

range of attraction forces. The results given in Fig. 8 show that
7 g/L of Glauber salt gives maximum exhaustion as compared to
table salt that inferred into high K/S value (Velmurugan et al.
2016; Ismal 2014). The reduction in amount of salt reveals that
microwave treatment is a cost-effective tool.
The results given in Fig. 9a, b for chemical mordanting
and Fig. 10a, b for bio-mordanting show that mordanting
has improved the color strength K/S and fastness proper-
ties. The chemical mordants used show that salts of alumi-
num and iron have given high color strength and darker
shades as compared to salts of Cu, Sn, and Co and tannic
acid. This is because aluminum and iron form firm metal
dye complex with un-irradiated cotton fabric (NRC) before
and after dyeing via good diffusion followed by coordinate
covalent interaction (Bouatay et al. 2016). The presence of
a conjugated system in alkaloids has made it more viable to
interact with metals like Al and Fe. Also, due to low re-
duction power of Fe and Al, the coordinate covalent inter-
action has shown more significant effect which upon dye-
ing resulted into darker shades. Similarly, the results for
bio-mordants show that due to the intermolecular H-
bonding between OH of colorants present in bio-
mordants and alkaloids, not only new shades are observed
but also high K/S is obtained. Comparative to chemical
mordant, bio-mordants have high K/S value which even
upon investigation to fastness agencies give fade resistance
property. The use of bio-mordants has made the dyeing
process more ecofriendly and effective eco-label (Ranu
et al. 2007; Hassan et al. 2017). From bio-mordants, acacia
has given darker shade due to availability of OH to make
H-bonding with fabric and colorant.
The rating results of fastness characteristics given in
Tables 1 and 2 and Tables 3 and 4 for pre- and post-
mordanted fabrics dyed at optimal conditions reveal that
MW treatment has improved the rating. This is because of
the formation of metal dye complex via metal salt and inter-
molecular H-bonding via bio-mordants (Prabhu and Bhute
2012; Haji 2012). The conjugated system present in colorant
and bio-mordants also adds value that upon exposure to light,
heat, detergents, and crocking were resistant to detach (Ismal
2017). Hence, depending upon the nature of colorants and
mordants, the role of MW treatment has been met to enhance
the coloring behavior of new harmal as a source of plant-based
natural dye.
Conclusion
Exploration of ecofriendly for green textile dyeing is
always a new task for researchers, traders, and consumers.
The awareness spread among global community has raised
the urge to use such dyed products owing to their green
benefits. The current study has been undertaken to explore
harmala seeds as a novel source of yellowish red natural
colorant for cotton dyeing using microwave treatment. It is
found that the extract obtained from 8 g powder followed
by microwave treated for 4 min in the acidified methanolic
medium has given good tint onto un-irradiated cotton fab-
ric. The acceptable characteristics have been obtained by
dyeing optimal fabric at 85 °C for 45 min of 7 g/L of
Glauber’s salt using 25 mL of irradiated dye bath of
pH 9. The addition of herbal bio-mordant has made the
process more ecofriendly and sustainable, where in com-
parison bio-mordants overall have shown great impact than
chemical mordants. It is concluded that microwave treat-
ment have great potential to explore the new dye yielding
plants for textile dyeing thereby making the dyeing process
more cost, time, and energy effective.
Acknowledgments We are thankful to Mr. Zafar Iqbal, Manager of Noor
Fatima Fabrics, Faisalabad, Pakistan, and Mr. Muhammad Abbas, Chief
Executive of Harris Dyes and Chemicals, Faisalabad, Pakistan, for giving
us the technical and scientific guidance at lab-scale experiments and for
providing us the facilities of fastener testers to conduct a part of PhD
studies. The current work is a part of PhD studies.

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