Increasing worldwide interest towards natural and sustainable products has driven the textile processing industry to use dyes and chemicals obtained directly from natural resources. Also, textile processors and researchers have been exploring the emerging technologies such as using ultrasonic energy, plasma, supercritical carbon dioxide, microwave and electrochemical methods for processing. In the same context, this work was undertaken to develop a method for dyeing of cotton fabric with natural dye extracted from marigold flower petals using ultrasonic energy. The aqueous extraction of natural dye from marigold flower petals was optimized for temperature and time. The resulting extract was used to further optimize its dyeing conditions on cotton fabric by ultrasonic and conventional exhaust dyeing methods. The effect of pre-mordanting with alum was also studied. Generally, all dyed samples were built with either yellow, golden yellow or tan colours (depending on varying dyeing parameters and conditions). It was found that the optimum aqueous extraction can produce strong colour yields with K/S value up to 5. Whereas, ultrasonic dyeing produced better colour yields comparing to conventional exhaust dyeing method. The colourfastness testing of optimum dyed fabric samples was also carried out for rubbing, washing and light exposure. The overall colourfastness of the dyed samples was acceptable except washing fastness of the sample dyed by conventional exhaust method without mordanting. However, washing fastness was considerably improved with pre-mordanting and further improved by ultrasonic dyeing method. Further, the rubbing and light fastness results were very good in case of pre-mordanting and ultrasonic dyeing method.

1. Ultrasonic Dyeing of Cotton with Natural Dye Extracted from
Marigold Flower
Awais Khatri, Sadam Hussain, Ameer Ali, Urooj Baig and Pashmina Khan
Department of Textile Engineering, Mehran University of Engineering and Technology, Jamshoro – 76060
Sindh Pakistan
Abstract. Increasing worldwide interest towards natural and sustainable products has driven the textile
processing industry to use dyes and chemicals obtained directly from natural resources. Also, textile
processors and researchers have been exploring the emerging technologies such as using ultrasonic energy,
plasma, supercritical carbon dioxide, microwave and electrochemical methods for processing. In the same
context, this work was undertaken to develop a method for dyeing of cotton fabric with natural dye extracted
from marigold flower petals using ultrasonic energy. The aqueous extraction of natural dye from marigold
flower petals was optimized for temperature and time. The resulting extract was used to further optimize its
dyeing conditions on cotton fabric by ultrasonic and conventional exhaust dyeing methods. The effect of pre-
mordanting with alum was also studied. Generally, all dyed samples were built with either yellow, golden
yellow or tan colours (depending on varying dyeing parameters and conditions). It was found that the
optimum aqueous extraction can produce strong colour yields with K/S value up to 5. Whereas, ultrasonic
dyeing produced better colour yields comparing to conventional exhaust dyeing method. The colourfastness
testing of optimum dyed fabric samples was also carried out for rubbing, washing and light exposure. The
overall colourfastness of the dyed samples was acceptable except washing fastness of the sample dyed by
conventional exhaust method without mordanting. However, washing fastness was considerably improved
with pre-mordanting and further improved by ultrasonic dyeing method. Further, the rubbing and light
fastness results were very good in case of pre-mordanting and ultrasonic dyeing method.
Keywords: Ultrasonic, Dyeing, Cotton, Natural dye, Marigold
1. Introduction
Due to global shift of industrial practices towards sustainable processing and products, use of natural
colorants has obtained a great attention. And, most of the natural colorants are non-toxic, non-carcinogenic
and biodegradable. However, the biggest challenge for dyeing textile materials with natural dyes is
reproducibility in presence of highly reproducible synthetic dyes. Therefore, textile processors and
researchers have been exploring a variety of natural colorants and using them by various techniques and
emerging technologies [1-2], for having a comparably reproducible natural dyeing processes. Natural colours
extracted from marigold flower, scientifically known as tagetes species, have been used as one of the
potential source of the yellow and brown natural dye for textile materials [3-6].
Use of ultrasonic energy to expedite the textile wet processes is one of the emerging technologies for
reducing energy consumption and wastewater pollution. A number of successful works have been reported
on ultrasonic-assisted dyeing of textile materials [7-11]. An industrial scale success on reactive dyeing of
cotton using ultrasonic energy has also been reported [12]. Ultrasonic-assisted dyeing of textile material with
natural dyes have shown an additional advantage of reducing energy consumption and reducing more
wastewater pollution [13-18].
Marigold plants are widely cultivated in Pakistan, and hence, are indigenous source of marigold flowers.
Moreover, marigold flower extracts have not been used for ultrasonic-assisted dyeing of textile materials yet.
Therefore, this work was undertaken to study the ultrasonic-assisted dyeing of cotton fabric with natural dye
extracted from marigold flower. The dye extraction process was optimised. Optimised extracts were used for
exhaust and ultrasonic dyeings of cotton fabric, and processes were optimised. The dyed fabric samples were
tested for colour yield and colourfastness.
2. Material and methods
ISBN xxx-x-xxxxx-xxx-x
The 13th
Asian Textile Conference
Geelong, Australia, November 3 - 6, 2015, pp. xxx-xxx

2. 2.1. Material
A mill scoured and bleached cotton woven fabric (150 g/m2
) was obtained from Gul Ahmed Textile
Mills Ltd. Karachi Pakistan. Fresh marigold flowers were purchased from local market in Hyderabad
Pakistan. The flower petals were taken off and mixed homogenously for extraction. The sodium chloride was
analytical and alum was commercial grades. Deionised water was used for all experiments.
2.2. Processes
Dye extraction. Homogenous mixture of flower petals were heated in water (petals-to-water ratio of
1:10) at varying temperatures (60 – 120 o
C) for varying time (30 – 105 min). For optimising extraction
temperature and time, ready-to-dye fabric samples were treated in the extract with the conditions: extract-to-
fabric ratio of 15:1, 50 g/L sodium chloride, temperature of 70 o
C for 30 min. The treated samples were
tested for colour yield (K/S value), the highest value was noted for the optimum extraction conditions.
Exhaust dyeing. Dyeing of fabric samples was carried out in the extract with extract-to-fabric ratio of
15:1 on an Rapid H.T. dyeing machine (H-120 Taiwan). The dyeing process was started at 40 o
C followed by
addition of sodium chloride (30 – 90 g/L) after 10 min. The process was continued for 15 min, then
temperature was raised to 45 – 105 o
C (dyeing temperature) and continued for 30 – 105 min (dyeing time).
Finally dyeing solution was drained and samples were rinsed thoroughly with running tap water.
Ultrasonic dyeing. Dyeing of fabric samples was carried out in the extract with extract-to-fabric ratio of
15:1 on a Getidy ultrasonic bath (KDC-200B China). The rest of the process steps same as those for exhaust
dyeing except the fixation temperature that was constant (80 o
C).
Mordanting. To study the effect of mordanting before dyeing (at optimum conditions), fabric samples
were treated with 1 – 5 % (on mass of fibre) of the alum at 60 o
C for 60 min. The solution-to-fabric ratio was
15:1.
2.3. Testing
Colour yield (K/S value at maximum absorption peak) of all dyed samples and CIE L* a* b* values of
the samples subjected to pre-mordanting were measured on an Xrite Spectrophotometer (CE7000 USA). The
optimum dyed samples were tested for colourfastness to mercury light (BS 1006: 1990 UK-TN), rubbing
(ISO-105: X12), and washing (ISO-105: CO2).
0
1
2
3
4
5
6
60 75 90 105 120
K/S
Extractiontemperature (oC)
0
1
2
3
4
5
6
30 45 60 75 105
K/S
Extractiontime (minutes)
Fig. 1: Effect of extraction temperature and time on colour yield of the dyed fabric.
3. Results and discussion
3.1. Optimization of extraction temperature and time
Figure 1 shows the effect of extraction temperature and time on colour yield (K/S) values of the fabric
samples dyed as per dyeing method for dye extraction mentioned in the section 2. Optimisation of
temperature was carried out at constant time (45 min) followed by optimisation of the time at optimum
temperature (90 o
C). The results show that colour yield was increased with increasing extraction temperature
and time up to a maximum level (i.e. 90 o
C and 60 min) then decreased with further increase. That may be
because more temperature and time over-cooked the extracted colour resulting in colour decomposition [19].

3. 3.2. Exhaust and ultrasonic dyeings
Effect of dyeing temperature and time. Results of the effect of exhaust dyeing temperature on colour
yield of the fabric dyed for constant time (60 min) is shown in Figure 2. The results show that the colour
yield increased up to 75 oC then decreased with increasing temperature. The increase in colour yield can
directly be attributed to the increase in dye exhaustion with increasing temperature. However, the decrease in
the colour yield at higher dyeing temperatures may be attributed to dyebath stability and colour
decomposition [19].
0
1
2
3
4
5
6
45 60 75 90 105
K/S
Dyeing temperature (oC)
Fig. 2: Effect of exhaust dyeing temperature on colour yield of the dyed fabric.
Figure 3 shows the effect of dyeing time on colour yield of the fabrics dyed at constant temperature
(75 o
C for exhaust dyeing and 80 o
C for ultrasonic dyeing). The optimum dyeing time for exhaust dyeing was
60 min and that for ultrasonic dyeing was 45 min. Moreover, ultrasonic dyeings produced considerably
higher colour yields comparing to those obtained by exhaust dyeings. The higher colour yield obtained in
lesser dyeing time may be attributed to the increased dye mobility due to continuous formation of cavitation
in the ultrasonic bath [7].
0
1
2
3
4
5
6
30 45 60 75 90 105
K/S
Dyeing time (min)
Exhaust dyeing
Ultrasonic dyeing
Fig. 3: Effect of exhaust and ultrasonic dyeing time on colour yield of dyed fabric in comparison
Effect of sodium chloride concentration. Sodium chloride was used as an electrolyte for promoting dye
exhaustion during dyeing. In Figure 4, colour yield values increase with increasing sodium chloride
concentration up to 70 g/L then decrease for both exhaust and ultrasonic dyeings. However, at optimum
values exhaust dyeing had slightly better effect of the concentration. This may be due to higher molecular
mobility in the ultrasonic bath.
Effect of mordanting. CIE L* a* b* values were preferred for this experiment because colour of the dyed
fabric can change by mordanting depending on the type and concentration of mordant. Effect of alum
(mordant) concentration on colourimetric values of the fabrics dyed by exhaust and ultrasonic dyeings is
given in Table 1. The results show that colour depth was increased with increasing alum concentration up to
4 %. After that there was a slight decrease in the depth. The hue values (CIE a* and b*) changed slightly
with changing alum concentration, however, the overall hue was yellowish brown. The CIE a* values were

4. very close to the central axis therefore had a greyish red effect whereas CIE b* values show dull yellow
effect, thus the overall hue appeared yellowish brown.
0
1
2
3
4
5
6
30 40 50 60 70 80 90
K/S
Sodium chloride concentration(g/L)
Exhaust dyeing
Ultrasonic dyeing
Fig. 4: Effect of sodium chloride concentration on colour yield of fabrics dyed by exhaust and ultrasonic dyeings
Table 1: Effect of alum concentration on CIE colour coordinates
Alum concentration
(%, on mass of fibre)
CIE Color Coordinates
Exhaust dyeing Ultrasonic dyeing
L* a* b* L* a* b*
0 70.13 3.22 13.07 68.01 3.13 13.01
1 69.82 3.09 12.61 68.70 3.00 12.76
2 68.69 2.80 12.46 67.83 2.75 12.31
3 68.63 3.22 11.93 63.16 3.13 11.21
4 63.78 3.28 10.21 63.00 3.30 10.93
5 64.13 3.30 9.23 67.43 3.91 10.82
3.3. Colourfastness results
The colourfastness results given in Table 2 show that the overall colourfastness of the dyed samples was
acceptable except washing fastness (change in colour) of the sample dyed by exhaust method without
mordanting. However, washing fastness was considerably improved with pre-mordanting by 2 units and
further improved by ultrasonic dyeing method by 0.5 unit. The wet rubbing of dyed samples was moderate
except pre-mordanted sample dyed by ultrasonic method. The dry rubbing was generally good. Further, the
lightfastness results were also generally good. The pre-mordanted samples dyed by ultrasonic method had
very good overall colourfastness.
Table 2: Colourfastness results of samples dyed with optimum conditions
Dyeing method
Rubbing fastness
(Grey scale rating)
Washing fastness (Grey
scale rating) Light fastness
(Blue wool
reference scale)Dry Wet
Colour
change
Staining
on cotton
Exhaust dyeing without mordanting 4 3 1/2 2/3 5
Exhaust dyeing with mordanting 4 3 3/4 4/5 5
Ultrasonic dyeing without mordanting 4/5 3 2 2/3 5
Ultrasonic dyeing with mordanting 4/5 4/5 4 4/5 6
4. Conclusions

5. Cotton fabrics could successfully be dyed with Marigold flower extracts. However, mordanting was
required to achieve acceptable colourfastness results. The dyeing of cotton fabrics with Marigold flower
extracts could also be carried out successfully using ultrasonic energy. Ultrasonic dyeings produced
considerably higher colour yields comparing to those obtained by exhaust dyeings in a lesser dyeing time.
The colourfastness results were also better in case of ultrasonic dyeings. The pre-mordanted samples dyed by
ultrasonic method had very good overall colourfastness. Moreover, energy required to heat-up the dyebath
can be saved in case of ultrasonic dyeings due to a fact that ultrasonic bath heats-up by itself due to
cavitation.
5. References
[1] M. Shahid, Shahid-ul-Islam, F. Mohammad, ‘Recent advancement in natural dye applications: a review’,
Journal of Cleaner Production, 53 (2013) 310-331.
[2] M. Banchero, ‘Supercritical fluid dyeing of synthetic and natural textiles – a review’, Coloration Technology,
129 (2012) 2-17.
[3] D. Jothi, ‘Extraction of natural dyes from african marigold flower (tagetes ereectal) for textile coloration’,
AUTEX Research Journal, 8 (2008) 49-53.
[4] M. Montazer, M. Parvinzadeh, ‘Dyeing of wool with marigold and its properties’, Fibers and Polymers, 8
(2007) 181-185.
[5] P. S. Vankar, ‘Chemistry of natural dyes’, Resonance, October (2000) 73-80.
[6] M. R. Katti, R. Kaur, N. Shrihari, ‘Dyeing of silk with mixture of natural dyes’, Colourage, 43 (1996) 37-39.
[7] S. A. Larik, A. Khatri, S. Ali, S. H. Kim, ‘Batchwise dyeing of bamboo cellulose fabric with reactive dye using
ultrasonic energy’, Ultrasonics Sonochemistry, 24 (2015) 178–183.
[8] C. Udrescu, F. Ferrero, M. Periolatto, ‘Ultrasound-assisted dyeing of cellulose acetate’, Ultrasonics
Sonochemistry, 21 (2014) 1477–1481.
[9] Z. Khatri, M. H. Memon, A. Khatri, A. Tanwari, ‘Cold pad-batch dyeing method for cotton fabric dyeing with
reactive dyes using ultrasonic energy’, Ultrasonics. Sonochemistry, 18 (2011) 1301-1307.
[10]M. M. Kamel, H. M. Helmy, H. M. Mashaly, H. H. Kafafy, ‘Ultrasonic assisted dyeing: dyeing of acrylic
fabrics C.I. Astrazon Basic Red 5BL 200%’, Ultrasonics Sonochemistry, 17 (2010) 92-97.
[11]M. M. Kamel, R. M. El-Shishtawy, H. L. Hanna, N. S. E. Ahmed, ‘Ultrasonic-assisted dyeing: I. Nylon
dyeability with reactive dyes’, Polymer International, 52 (2003) 373-380.
[12]K. A. Thakore, ‘Ultrasound Treatment in Exhaust and Pad-Batch Dyeing’, AATCC Review, July-August
(2011) 66-74.
[13]A. Guesmi, N. Ladhari, F. Sakli, ‘Ultrasonic preparation of cationic cotton and its application in ultrasonic
natural dyeing’, Ultrasonics Sonochemistry, 20 (2013) 571–579.
[14]M. M. Kamel, M. M. El Zawahry, N. S. E. Ahmed, F. Abdelghaffar, ‘Ultrasonic dyeing of cationized cotton
fabric with natural dye. Part 1: Cationization of cotton using Solfix E’, Ultrasonics Sonochemistry, 16 (2009)
243-249.
[15]M. M. Kamel, H. M. Helmy, N.S. El-Hawary, ‘Some studies on dyeing properties of cotton fabrics with crocus
sativus (saffron) (flowers) using an ultrasonic method’, AUTEX Research Journal, 9 (2009) 29-35.
[16]M. M. Kamel, R. M. El-Shishtawy, B. M. Youssef, H. Mashaly, ‘Ultrasonic assisted dyeing. IV. Dyeing of
cationised cotton with lac natural dye’, Dyes and Pigments, 73 (2007) 279-284.
[17]P. S. Vankar, R. Shanker, J. Srivastava, ‘Ultrasonic dyeing of cotton fabric with aqueous extract of Eclipta
alba’, Dyes and Pigments, 72 (2007) 33-37.
[18]M. M. Kamel, R. M. El-Shishtawy, B. M. Yussef, H. Mashaly, ‘Ultrasonic assisted dyeing: III. Dyeing of wool
with lac as a natural dye’, Dyes and Pigments, 65 (2005) 103–110.
[19] Shaukat Ali, Tanveer Hussain, Rakhshanda Nawaz, ‘Optimization of alkaline extraction of natural dye from
Henna leaves and its dyeing on cotton by exhaust method’, Journal of Cleaner Production, 17 (2009) 61–66.

6. Cotton fabrics could successfully be dyed with Marigold flower extracts. However, mordanting was
required to achieve acceptable colourfastness results. The dyeing of cotton fabrics with Marigold flower
extracts could also be carried out successfully using ultrasonic energy. Ultrasonic dyeings produced
considerably higher colour yields comparing to those obtained by exhaust dyeings in a lesser dyeing time.
The colourfastness results were also better in case of ultrasonic dyeings. The pre-mordanted samples dyed by
ultrasonic method had very good overall colourfastness. Moreover, energy required to heat-up the dyebath
can be saved in case of ultrasonic dyeings due to a fact that ultrasonic bath heats-up by itself due to
cavitation.
5. References
[1] M. Shahid, Shahid-ul-Islam, F. Mohammad, ‘Recent advancement in natural dye applications: a review’,
Journal of Cleaner Production, 53 (2013) 310-331.
[2] M. Banchero, ‘Supercritical fluid dyeing of synthetic and natural textiles – a review’, Coloration Technology,
129 (2012) 2-17.
[3] D. Jothi, ‘Extraction of natural dyes from african marigold flower (tagetes ereectal) for textile coloration’,
AUTEX Research Journal, 8 (2008) 49-53.
[4] M. Montazer, M. Parvinzadeh, ‘Dyeing of wool with marigold and its properties’, Fibers and Polymers, 8
(2007) 181-185.
[5] P. S. Vankar, ‘Chemistry of natural dyes’, Resonance, October (2000) 73-80.
[6] M. R. Katti, R. Kaur, N. Shrihari, ‘Dyeing of silk with mixture of natural dyes’, Colourage, 43 (1996) 37-39.
[7] S. A. Larik, A. Khatri, S. Ali, S. H. Kim, ‘Batchwise dyeing of bamboo cellulose fabric with reactive dye using
ultrasonic energy’, Ultrasonics Sonochemistry, 24 (2015) 178–183.
[8] C. Udrescu, F. Ferrero, M. Periolatto, ‘Ultrasound-assisted dyeing of cellulose acetate’, Ultrasonics
Sonochemistry, 21 (2014) 1477–1481.
[9] Z. Khatri, M. H. Memon, A. Khatri, A. Tanwari, ‘Cold pad-batch dyeing method for cotton fabric dyeing with
reactive dyes using ultrasonic energy’, Ultrasonics. Sonochemistry, 18 (2011) 1301-1307.
[10]M. M. Kamel, H. M. Helmy, H. M. Mashaly, H. H. Kafafy, ‘Ultrasonic assisted dyeing: dyeing of acrylic
fabrics C.I. Astrazon Basic Red 5BL 200%’, Ultrasonics Sonochemistry, 17 (2010) 92-97.
[11]M. M. Kamel, R. M. El-Shishtawy, H. L. Hanna, N. S. E. Ahmed, ‘Ultrasonic-assisted dyeing: I. Nylon
dyeability with reactive dyes’, Polymer International, 52 (2003) 373-380.
[12]K. A. Thakore, ‘Ultrasound Treatment in Exhaust and Pad-Batch Dyeing’, AATCC Review, July-August
(2011) 66-74.
[13]A. Guesmi, N. Ladhari, F. Sakli, ‘Ultrasonic preparation of cationic cotton and its application in ultrasonic
natural dyeing’, Ultrasonics Sonochemistry, 20 (2013) 571–579.
[14]M. M. Kamel, M. M. El Zawahry, N. S. E. Ahmed, F. Abdelghaffar, ‘Ultrasonic dyeing of cationized cotton
fabric with natural dye. Part 1: Cationization of cotton using Solfix E’, Ultrasonics Sonochemistry, 16 (2009)
243-249.
[15]M. M. Kamel, H. M. Helmy, N.S. El-Hawary, ‘Some studies on dyeing properties of cotton fabrics with crocus
sativus (saffron) (flowers) using an ultrasonic method’, AUTEX Research Journal, 9 (2009) 29-35.
[16]M. M. Kamel, R. M. El-Shishtawy, B. M. Youssef, H. Mashaly, ‘Ultrasonic assisted dyeing. IV. Dyeing of
cationised cotton with lac natural dye’, Dyes and Pigments, 73 (2007) 279-284.
[17]P. S. Vankar, R. Shanker, J. Srivastava, ‘Ultrasonic dyeing of cotton fabric with aqueous extract of Eclipta
alba’, Dyes and Pigments, 72 (2007) 33-37.
[18]M. M. Kamel, R. M. El-Shishtawy, B. M. Yussef, H. Mashaly, ‘Ultrasonic assisted dyeing: III. Dyeing of wool
with lac as a natural dye’, Dyes and Pigments, 65 (2005) 103–110.
[19] Shaukat Ali, Tanveer Hussain, Rakhshanda Nawaz, ‘Optimization of alkaline extraction of natural dye from
Henna leaves and its dyeing on cotton by exhaust method’, Journal of Cleaner Production, 17 (2009) 61–66.