Fibers and Polymers 2007, Vol.8, No.

2, 181-185

Dyeing of Wool with Marigold and Its Properties

M. Montazer * and M. Parvinzadeh1

Textile Department, Amirkabir University of Technology, Tehran, Iran
1
Institute for Colorants, Paint and Coating, Tehran, Iran
(Received October 16, 2006; Revised January 25, 2007; Accepted February 19, 2007)

Abstract: This research work involves the dyeing of wool with Marigold as a source of yellow colour. To do this, wool yarns
pre-treated with Alum as a colorless mordant, dyed with Marigold and then treated with different percentages of ammonia
solutions. The chromaticity co-ordinates of samples measured in CIELAB system. The L* values of all ammonia treated sam-
ples decreased and the values of a*, b*, C* dependant on the ammonia solution. It can also indicate that the reflectance spec-
trum of treated samples decreases due to ammonia treatment. The rate of vertical wicking decreases on Marigold dyed treated
with ammonia. Color hue of the Marigold dyed wool alters after washing with standard soap and ammonia after-treatment
has no influence on washing fastness. The samples dyed with Marigold and after-treated with ammonia show a lower light
fastness.
Keywords: Wool, Marigold, Dyeing, Ammonia, Chromaticity co-ordinates

Introduction and for adorning buildings and statues of spiritual significance

Natural dyes of plant origin are present in plants as aglycones
or glycosides which are free or bound to sugars [1]. Natural
dyes seem to be less harmful on humans and environment,
and nowadays they could be considered as a better alternative to
synthetic dyes [2-8].
Marigold is a plant of the genus Tagetes of the family
Asteraceae, mostly cultivated as garden flower that is one of
the natural sources for achieving yellow color. Marigolds
were well known and valued by ancient people in South Asia.
Their golden colour was considered to resemble the colour
of the Arya, or honourable people. It was used to demarcate
special spaces like pavilions and to line sacred fire-pits or
kunds in which ceremonies were performed [9,10]. Picture
of Marigold illustrated in Figure 1.
Currently, Marigold plants are grown for pigment production
in Mexico, Peru, and India. From decoration to dyes, brightly
coloured yellow and orange Marigolds provide familiar splashes
of colour in South Asia. They are mainly used to make garlands
but have also been used to make skin creams. In Britain,
Marigold planted by gardeners to discourage pests. The essential
oil from the leaves of this flower has been reported to have
some anti-fungal and insecticidal properties [9,10].
Marigold flowers are used at many religious ceremonies
and festivals. Strung together they make colourful garlands
and are used as offerings and to decorate religious buildings
and statues. The petals are used in South Asia to dye fabrics
and wool yarns [10]. Marigold plants are stout and branching
and can grow up to 60 cm tall. Leaves of Marigold are dark
green in colour and are strongly scented. Flowers vary in
colour from yellow and gold to orange, red and mahogany.
The taller and larger-flowered Tagetes erecta was often
called African Marigold and the smaller Tagetes patula was
known as French Marigold. But Marigolds have been cultivated
all over the world and lots of similar hybrid varieties have
been developed from the two species [11,12].
Marigold flowers contain compounds called carotenoids.
Lutein (C H O ) is a natural pigment of the carotenoid family.
40 56 2

It is widely found in nature. Lutein and its isomer zeaxanthin

Figure 1. Marigold (Calendula officinalis).
*Corresponding author: tex5mm@aut.ac.ir
also known as oxycarotenoids. They are the main xanthophylls
in Marigold flowers and also in vegetables such as spinach
and kale. It is also present in foods such as corn and egg yolks
and can be found in the eye, skin, cervix and the breast. It
is a powerful antioxidant and helps in maintaining healthy
eyes [9,13].
Lutein includes alpha- and beta-cryptoxanthin, contains
hydroxyl groups. This makes it more polar than other carot-
enoids, such as beta-carotene and lycopene, which do not
contain oxygen. Although lutein has identical chemical formulas
and is isomer, it is not stereoisomers, as is sometimes believed.
It is polyisoprenoid containing 40 carbon atoms and cyclic
structures at each end of its conjugated chains. Also, it occurs
naturally as all-trans (all-E) geometric isomers [13,14].
In the green parts of the plants, in fruits and in seeds, Lutein

181
182 Fibers and Polymers 2007, Vol.8, No.2
is found in its free form, meaning that it does not have any
other types of molecules attached to it. On the other hand,
Lutein found in flower petals of Marigold and is chemically
bound to various types of fatty acids. It is believed that, lutein is
esterified and is commonly known as Lutein Ester [13,14].
Marigold flowers are manufactured from the dried flower
petals. These are extracted according to high standard specifi-
cations. The Marigold extract is heated to increase flow ability
and then purified to remove the fatty acids commonly found
in Marigold extract. These extracts are used as a food coloring
for humans and livestock [14]. Lutein, a major carotenoid
compound existed in Marigold.
Many research papers have been published on fastness
properties of natural dyes but few research papers dealing with
alteration of the color with pH. It was showed that the sensitivity
of the natural pigments to pH occur on the deacidification
treatment of water color pigments. It was suggested that
structural change in chromophore system of dyes caused by
changes in pH and this phenomenon occur during cleaning
treatment [15]. Treatment of Marigold dyed wool with ammonia
may introduce the yarns with new properties and probably
the fiber with structural changes (bulking effect) [16]. We have
already investigated dyeing of wool with pomegranate shells,
madder, cochineal, walnut, weld, white onion and red onion and
also examined the effect of ammonia after-treatment [17-19].
In this paper dyeing of wool with marigold and alteration of
colour after-treated with ammonia examined and reported.
Experimental
Materials
Iranian wool yarns of 432/2 Tex with 144 twist per meter
and nonionic detergent was supplied from Iranian Carpet Co.
Standard washing soap was purchased from SDL representative
in Iran. Analytical grade of 85 % formic acid, aluminium
potassium sulfate and 25 % ammonia from Merck was used.
And the flowers of Marigold prepared from Fars province.
Procedure
The wool yarns were first scoured with 0.5 % nonionic
detergent in the bath with L:G (liquor to good ratio) of 40:1 for
30 min at 50 C. The scoured wool were then mordanted with
o
20 % o.w.f. AlK(SO ) at L:G of 40:1. Formic acid was used
4 2
for adjusting the pH 5. The mordanting started at 40 C and o
rose to boil over 20 min and remained at the boil for 1 h. The
dye solution were prepared 24 h before dyeing by adding the
flowers of Marigold to water (Marigold:water=10:1). The
dyeing bath prepared by adding 50 % ow.f of dye solution,
pH of 5 with formic acid and L:G of 40:1. Dyeing was
started at 40 C and temperature raised to 85 C over 20 min
o o
and held for 1 hour. Treatment with ammonia solution was
carried out after dividing the dyed samples into four parts.
One part was retained for reference and the others were each
treated with ammonia solution (1 %, 3 % and 5 % w/w) at
M. Montazer and M. Parvinzadeh
25 C for 10 min and L:G of 20:1.
o
The reflectance spectra of the dyed samples evaluated
using a Spectrophotometer Color-eye 7000A integrated with
an IBM-PC. CIELAB color coordinates (L , a , b , C , h)
* * * *
and reflectance spectra of the dyed samples were calculated
for 10 observer and illuminant D65.
o
Vertical wicking of the raw, scoured, mordanted and Marigold
dyed yarns treated with ammonia were also examined. For
this purpose, each sample was hung vertically over the water
container and 1 cm of the sample soaked in water. After
1 min, the wet height of the samples was measured by means
of a ruler.
The wash-fastness of the Marigold dyed yarns were measured
according to ISO 105-C01. The degree of staining on the
adjacent yarns was measured after drying.
For light-fastness measurements, the yarns were exposed
to the daylight for 7 days according to the daylight ISO 105-
B01, and the changes in the color (fading) were assessed by
the blue scale.
Results and Discussion
Colour Measurement
The complex produced by wool protein, the lutein, a major
carotenoid compound present in Marigold, and aluminium
salt is illustrated in Figure 2(a). The changes occurring in the
complex after treatment with ammonia is proposed in Figure
2(b).
The color hue of the Marigold-dyed yarns was changed and
a small amount of Marigold bled from the dyed yarns after
treated with ammonia. The change in color hue of Marigold
was also observed in the remaining ammonia solution. It can
be seen from Figure 3 that an increase in the concentration of
ammonia on the Marigold dyed wool yarns leads to prolonged
decrease of reflectance spectra at different wavelengths.
The results of color measurement of ammonia-treated wool
yarns dyed with Marigold are shown in Table 1 and Figures 4
and 5. It can be seen from Figures 4 and 5 that the amount of
L decreases after the Marigold dyed sample treated with 1 %
*
ammonia solution but the amount of a (redness) increases.
*
By increasing the percentage of ammonia, the amount of L *
and a continued to decrease and increase, respectively.
*
According to Figure 5, the corresponding b value increases
*
due to ammonia treatment. It can be also observed (Table 1)
that the C value for Marigold dyed sample increases after
*
ammonia treatment that means the shade became brighter.
Vertical Wicking Test
The results of vertical wicking tests are shown in Figures 6-8.
It can be seen from Figure 6 that wicking increases with
scouring; this was intensified by the additional treatment of
ammonia. Also the wicking rate increases with an increase
in the ammonia concentration. This means that the scouring
process can remove some of the impurities from the fiber
Dyeing of Wool with Marigold and Its Properties Fibers and Polymers 2007, Vol.8, No.2 183

Figure 2. (a) Complex of wool protein, molecule of lutein, and aluminium salt and (b) chemical structure of complex of wool protein, lutein,
and aluminium salt after treatment with ammonia.

Table 1. Color co-ordinates of ammonia treated and untreated

Marigold dyed wool
Ammonia
Dye concentration L* a* b* C* h
0% 56.29 3.95 36.93 37.14 83.88
1% 52.12 6.35 46.06 46.5 82.14
Marigold 3% 43.62 14.18 43.52 45.77 71.95
5% 41.14 14.36 40.96 43.41 70.68

and ammonia treatment then could help to remove the remain-

ing impurities. Removal of any impurities from the fibers
Figure 3. Reflectance spectra of ammonia treated and untreated increases the water absorption and the wicking can be done
Marigold dyed wool at different wavelengths. more easily and quickly. The results shown in Figure 7 indicate
184 Fibers and Polymers 2007, Vol.8, No.2 M. Montazer and M. Parvinzadeh

Figure 8. Vertical wicking of Marigold-dyed and Marigold-dyed/

Figure 4. L* values of Marigold-dyed and Marigold dyed/ammonia- ammonia-treated wool with 1, 3, and 5 % ammonia.
treated wool.
that mordanting of scoured yarns may have an influence on
the wicking and decrease wicking. It can be concluded from
Figure 8 that the wicking decreases by the ammonia treatment
on the Marigold-dyed yarn. A greater decrease of wicking can
be seen by increasing the ammonia concentration. It seems that
the ammonia treatment on the Marigold-dyed wool helps to
establish more complexes between dye and wool which leads
to less availability of hydrophilic groups, such as hydroxyl
groups, and decreases the absorbency of wool yarn.
Wash Fastness
Figure 5. a and b values of Marigold-dyed and Marigold-dyed/
* * There are no differences between the results of wash-fastness
ammonia-treated wool. for untreated and ammonia-treated dyed yarns (Table 2). It
should be mentioned that by treating the dyed samples with
standard soap during wash fastness test, the color hue of
Marigold-dyed yarns changed toward the visible wavelength.
Therefore, no more colour alteration observed on the samples
treated with 5 % ammonia solution.
Light Fastness
After exposing the samples to daylight for 2 days, the color

Table 2. Wash fastness of Marigold dyed and Marigold dyed/

ammonia treated wool
Figure 6. Vertical wicking of raw, scoured, and treated wool with Dye Ammonia Staining on Staining Wash
1, 3, and 5 % ammonia. concentration cotton on wool fastness
0% 5 4.5 4.5
1% 5 4.5 4.5
Marigold 3% 5 4.5 4.5
5% 5 4.5 4.5

Table 3. Light fastness of Marigold dyed and Marigold dyed/

ammonia treated wool
Dye Ammonia Light fastness Light fastness
concentration after 2 days after 7 days
0% 5 5
1% 3 3
Marigold 3% 3 3
Figure 7. Vertical wicking of raw, scoured, and mordanted wool
with AlK(SO4)2. 5% 2 2
Dyeing of Wool with Marigold and Its Properties
of Marigold-dyed yarns faded. An extension of the duration
of exposure to the daylight for 7 days, has no influence on
fading. This indicated that the color fading of the Marigold-
dyed yarns was limited to a certain period of exposure to
daylight. The results of light-fastness show (Table 3) that the
light-fastness of Marigold-dyed yarns treated with ammonia
are lower than untreated one and the ammonia treatment has
no positive effect on it. Carotenoid structure of lutein in
Marigold has substituents as hydroxyl groups (-OH) which
protects the dye structure against the ultraviolet radiation of
light. Ammonia treatment can alter the chromophoric structure
of the lutein and decreases the hydroxyl substituent groups
in the dye molecule and then the protective effects of these
groups decrease.
Conclusion
The color hue of Marigold-dyed yarns altered with ammonia
after treatment and the reflectance spectra over the wavelength
of 400 nm-700 nm decreases. The L value showed a decrease
*
after the Marigold dyed sample treated with 1 % ammonia
solution but a value (redness) increased. By increasing the
*
percentage of ammonia, the value of lightness and redness
continue to change. According to C values, the shade of
*
Marigold dyed samples treated with ammonia are brighter.
The wicking rate also decreases by ammonia treatment on
the Marigold-dyed yarn. Also there is no difference between
the wash-fastness of untreated and the ammonia-treated dyed
yarns. The color of the Marigold-dyed wool was changed after
wash-fastness test. This created a color hue on the samples
with higher absorbance. The results of the light-fastness also
showed a fading of the Marigold-dyed yarns.
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