atc13 full manuscript - engr sadam hussain- final version

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. IntroductionDue 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-xThe 13th Asian Textile Conference

Geelong, Australia, November 3 - 6, 2015, pp. xxx-xxx

2.1. MaterialA 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. ProcessesDye extraction. Homogenous mixture of flower petals were heated in water (petals-to-water ratio of

1:10) at varying temperatures (60 – 120 oC) 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 oC 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 oC 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 oC (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 oC).

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 oC for 60 min. The solution-to-fabric ratio was 15:1.

2.3. TestingColour 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

Extraction temperature (oC)

0

1

2

3

4

5

6

30 45 60 75 105

K/S

Extraction time (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 timeFigure 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 oC). The results show that colour yield was increased with increasing extraction temperature and time up to a maximum level (i.e. 90 oC 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].

3.2. Exhaust and ultrasonic dyeingsEffect 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 oC for exhaust dyeing and 80 oC 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 dyeingUltrasonic 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

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 dyeingUltrasonic 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 13.011 69.82 3.09 12.61 68.70 3.00 12.762 68.69 2.80 12.46 67.83 2.75 12.313 68.63 3.22 11.93 63.16 3.13 11.214 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 resultsThe 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

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.