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PII: S0959-6526(13)00169-8
DOI: 10.1016/j.jclepro.2013.03.031
Reference: JCLP 3368
Please cite this article as: Shahid M, Shahid-ul-Islam , Mohammad F, Recent advancements in natural
dye applications: A review, Journal of Cleaner Production (2013), doi: 10.1016/j.jclepro.2013.03.031.
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*Corresponding author
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Department of Chemistry,
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New Delhi-110025, India
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Phone: +91-9350114878. E-mail: faqeermohammad@rediffmail.com
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Abstract
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A vast array of colorants obtained from natural sources such as plants, insects/animals
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and microbes have been scrutinized in recent past for their use in different kinds of
applications. Research into new natural dyes sources along with eco-friendly, robust and cost-
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effective technologies for their processing and application have greatly aided in widening the
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scope of natural dyes in various traditional and advanced application disciplines. This review
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in natural textile dyeing and use of natural dyes in functional finishing of textiles, food
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coloration and dye sensitized solar cells. In addition, some newly discovered applications of
Keywords: Natural Dyes; Mordants; Protective textiles; Dye Sensitized Solar Cells; Food
coloration
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1. Introduction
With the publics enhanced cognizance to eco-safety and health concerns, environmentally
benignant and non-toxic bioresource products are regaining popularity in different spheres of
our lives. Natural dyes, obtained from plants, insects/animals and minerals, are renewable and
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sustainable bioresource products with minimum environmental impact and known since
antiquity for their use, not only in coloration of textiles (Kadolph, 2008) but also as food
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ingredients (Dweck 2002) and cosmetics (Frick, 2003). With the discovery of synthetic
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colorant mauve by W. H. Perkin in 1856 and subsequent upsurge in research, production
and application of synthetic dyes, use of natural colorants slumped sharply (Holme, 2006).
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However, the application of a number of synthetic dyes has detrimental effects on
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environment and associated allergic, toxic, carcinogenic, harmful responses. Amidst growing
synthetic dyes (Yusuf et al., 2011; Mirjalili et al., 2011). Recent resurgence in research and
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popularity of more natural lifestyle based on naturally sustainable goods (Grifoni et al.,
2009). Natural flora/fauna is full of exquisite colors fascinating and attracting human being
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towards a vast portfolio of possibilities (Dawson et al., 2009). A large number of plant and
animal/insect sources have been identified for extraction of color (Guinot et al., 2006; Kumar
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and Sinha, 2004) and their diversified use in textile dyeing (Samanta and Agarwal, 2009) and
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functional finishing (Gupta et al., 2005), food coloration (Delgado-Vargas, 2000), cosmetics
(Dweck 2002), Dye-sensitized solar cells (Hao et al., 2006), histological staining (Tousson,
and Al-Behbehani, 2011), pH indicator (Mishra et al., 2012) and several other application
disciplines (Kushwandi et al., 2012; Zyoud et al., 2011). During the last few decades,
increasing attention has been paid by researchers to various aspects of natural dye
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applications (Fig. 1) and extensive R&D in this area is underway worldwide. This review
article is intended to collect the dispersed information, from 1998 to 2013, about the recent
developments in traditional and newly discovered applications of natural dyes. Special focus
has been given to the technological development in natural textile dyeing and use of natural
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dyes in functional finishing of textiles, food coloration and dye sensitized solar cells.This
review article also highlights a number of issues which should be targeted to make natural
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dyes a viable co-partner/alternative to synthetic dyes.
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2. Technological advancements in textile coloration with natural dyes
Coloration is an integral part of ever expanding complex chemical wet processing of textiles,
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which involves use of many types of chemical entities and physico-chemical processes.
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Environmental concerns arising due to accelerated development in textile wet processing
industry paved the way for ongoing interest in the development of cleaner production
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strategies for making cost effective value added textile products (Ahmed and El-Shishtawy,
2010).
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Hill (1997), while discussing lack of quality research work on natural dyeing techniques
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cited, Our knowledge of dyeing techniques and recipes is gleaned from printed books and
dye house records and can be reconstructed and adapted. In last fifteen years, investigations
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about possible use of natural dyes in textile dyeing processes performed by various research
groups have changed the scenario to greater extent and relatively superior and sophisticated
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Natural dyeing in textiles is currently of great interest in both research fields as well as textile
industries due to increasing attention to the aspects of water pollution, sustainability of raw
(Bechtold et al., 2009). Studies on dyeing techniques were attempted by using both
conventional exhaustion method (Ali et al., 2009) as well as non-conventional methods such
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as ultrasonic (Kamel et al., 2005), microwave (Nourmohammadian and Gholami, 2008), pad
Pressure (HTHP) dyeing (Bhattacharya and Lohiya, 2002), contact dyeing (Kadolph and
Casselman, 2004) and other optimized methods. As a result, many research articles have been
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published dealing with re-establishment of traditional dyeing techniques (Mikropoulou et al.,
2009; Zarkogianni et al., 2011), variabilities of natural sources for dyeability (Bhuyan and
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Saikia, 2005; Sharma et al., 2012a), processing improvement for natural colorant extraction
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(Bechtold et al., 2002; Sivakumar et al., 2011), approaches to the improvement of color
fastness or dyeing characteristics for the naturally dyed fabrics, adaptation and optimization
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of natural dyeing methods and use of modern day technologies in different stages of natural
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textile dyeing process (Nasirizadeh et al., 2012; Samanta, and Agarwal, 2009). Any process
based on use of natural dyes will have to consider the environmentally sound processing
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techniques and the overall process must be competitive with regard to the use of chemicals,
energy, wastes and waste water and overall costs (Bechtold and Mahmud-Ali, 2008).
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Dyeing of fabrics with natural dyes often leads to problems such as narrow shade range, and
lower color fastness of the dyed textiles. Attempts to overcome these problems have been
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mainly focused on the use of mordants. In addition to creating affinity between dye and fibre,
the use of mordants also change the hue of certain dyes. Different mordants used with the
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same dye may darken, brighten or drastically alter the final color of the dyed fibre (Manhita
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et al., 2011; Yi and Cho, 2008). Colorimetric properties of the dyed fabrics such as Lightness
(L*), redness-yellowness (a*), blueness- greenness (b*), chroma (c*), hue (ho) and colour
strength (K/S) are greatly dependent on the chemical nature of mordants and fibers and the
metal ion complex forming ability with the dye and the fiber (Tang et al., 2010). Mordanting
generally improved dye performance and help the dyer to achieve a broad spectrum of colors
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on a wide range of natural as well as synthetic fibres with expanded shade ranges and better
fastness properties (Kadolph and Casselman, 2004). Samanta and Agarwal (2009) presented a
methods and their effects on natural dyeing for a variety of textile materials. Most commonly
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used mordants in natural dyeing are aluminium potassium sulfate, potassium dichromate,
stannous chloride, ferrous sulphate and copper sulfate (Samanta and Agarwal, 2009).
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Improving traditional mordanting processes and selecting new mordants to replace traditional
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heavy-metal ions has been an important part in the development of natural dyeing of textiles.
Several other metallic salt mordants were also attempted with satisfactory results on lab scale
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(Table 1). Zheng et al. (2011) have successfully employed rare earth chlorides as mordant for
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the dyeing ramie fabrics with natural dyes. Results showed that rare earth metals would be a
kind of promising environment friendly mordants in natural dyeing in comparison with the
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commonly used metallic salts in the present era of environment consciousness, as using rare
earth chlorides as mordants greatly reduced the ionic concentration in natural dyeing.
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Natural dyeing processes typically generate wastewater containing residual toxic metal ions
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from metal salt mordants which have negative impact on the environment and public health
(Burkinshaw and Kumar, 2009; Zheng et al., 2011). The content of metal ions in textile
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products and effluent discharged from textile industries is strictly prohibited beyond a certain
specified limit. Alum and ferrous sulphate are considered safest among metallic salt mordants
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and tin can be used up to certain limits while use of chrome and copper is almost banished
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considering their toxic nature (Savvidis et al., 2013; Zarkogianni et al., 2010). While dyeing
with natural dyes, a substantial proportion of mordant remains unexhausted in the residual
dyebath and thus may pose serious effluent problems, hence, it is important to pay special
attention to the limit values of metal ions in textiles and effluents prescribed by
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metallic salt mordants is also advised by some researchers. Although, the concept of natural
mordanting is not new; yet the lack of well documented research records on their application
downplays their role in real time natural textile dyeing. Biomordant sources are either plants
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with high tannin content (Prabhu and Teli, 2011) or metal hyperaccumulating plants
(Cunningham et al., 2011). Recently chlorophyll extracted from different plant sources has
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also been successfully employed as biomordant (Guesmi et. al., 2012). Vegetable tannins are
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water soluble polyphenolic compounds found in wide variety of plant parts such as bark
wood, fruit, fruit pods, leaves, roots and plant galls. Phenolic hydroxyl groups of tannins
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enable them to form effective crosslinks with different types of fibers and dyes and help in
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color fixation. Tannin based mordants were found most effective in case of cotton fibre
which has very low affinity for most of the natural dyes (Prabhu and Teli, 2011).
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Cunningham et al. (2011) presented a detailed review on reasons for selecting different Al-
hyperaccumulating plants as natural metallic mordants and their application in natural dyeing
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of traditional Indonesian textiles and its impact on religious, social and economic scenario.
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resource management for effective utilization of several other possible sources of Al-
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(2008d) observed that Euriya acuminata when used as mordant in conjunction with Rubia
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cordifolia dye was found to enhance the dyeability of silk fabric by chelation due to the high
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Al content present in their leaves. In another study Cu-hyperaccumulating plant Pyrus pashia
have been reported to provide better dye adherence due to stronger and useful chelation to the
flavone/flavonol dyes extracted from Delonix regia (Vankar et al., 2009). Use of metal
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which should be popularized as an alternate method that may help to reduce the reliance on
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The use of enzymes in textile industry is an example of industrial biotechnology, which
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strategies to improve the quality of final product. Different types of enzymes are commonly
used in various stages of textile processing for modification of physical and chemical surface
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properties or introduction of functional groups on the surface of textile fibres (Duran and
Duran, 2000; Jo et al., 2008). Many different approaches have been taken to the preparation,
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dyeing and finishing of cotton (Vankar and Shanker, 2008), wool (Montazer et al., 2009), silk
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(Vankar et al., 2007b; Vankar and Shanker 2009) and other textile fibres (Sricharussin, 2009)
with natural colorants using different types of enzymes. Tsatsaroni and co-authors used -
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amylase, amyloglycosidase and trypsin enzymes for preparation of cotton and wool samples
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for dyeing with saffron and curcumin (Kyriakides et al., 1998; Tsatsaroni et al., 1998). They
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have reported that enzymatic treatment resulted in improvement in dye uptake in all cases,
and attributed it to enhanced shrink-resistance properties of the treated fibres. Kumbasar et al.
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(2009) studied effects of alkali proteases on dyeing properties of various proteinous materials
with hydrolysable tannin based natural dyes obtained from sumac, myrobalan fruit, oak bark
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and gall nut and reported significant increase in dye uptake after enzymatic treatment.
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Madder dyed wool fabrics treated with protease (Parvinzadeh, 2007) and laccase (Montazer
et al., 2009) have shown higher water drop absorption, lower felting shrinkage, reduced
fabric weight and lower values of a*, b* and lightness without any change in fastness
properties of dyed samples. Vankar and co-authors studied effect of three enzymes lipase,
granatum, Rheum emodi (Vankar et al., 2007b), Acacia catechu, Tectona grandis and
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Delonix regia (Vankar and Shanker, 2008, 2009) on different types of textile fabrics. The
authors observed that enzymatic treatment gives rapid dye adsorption kinetics and total
higher adsorption than untreated samples in all the cases. The CIELab values also showed
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important factor in enhancing dyeing properties: protease-amylase combination is suited for
Acacia and Terminalia; lipase is suited for Rheum and Delonix, while diasterase is suited for
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Tectona and Punica. Compared to untreated wool, treatments with protease and
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transglutaminase enhanced K/S value of wool dyed with sappan dye; however no significant
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Although studies of enzymes used in natural textile dyeing (Table 3) have received limited
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attention in scientific literature, however, from the point of view of processing improvement,
possibilities for the development of new enzyme-based natural dyeing systems for a more
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eco-friendly approach in the textile industry, however further in depth research is needed
regarding dye enzyme compatibility for the choice of enzyme with a particular dye in order to
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The application of ultrasound power to textile dyeing has a significant role in the concept of
clean technology for textile processing. Ultrasound can improve effectiveness of a wide
variety of chemical and physical processes, mainly by generating cavitation in liquid medium
in addition to other mechanical effects such as dispersion, degassing, diffusion, and intense
agitation of liquid (Ahmed and El-Shishtawy, 2010). Cavitation is the formation, growth, and
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compression and rarefaction waves. The cavitation bubbles oscillate and implode, thus
enhancing molecular motion and stirring effect in the dye bath. When cavitation occurs at a
produces micro streaming towards the solid surface which greatly disrupts the diffusion
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interlayer and promotes mass transport in that direction (Vankar et al., 2008a,b). Cavitation
and its physicochemical consequences enhance the dyeing rate; economize energy and time
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consumption without causing any apparent fibre damage (Vankar and Shanker, 2008). In the
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last few years a certain number of studies on ultrasound assisted natural dyeing and finishing
of natural and synthetic fibres were carried out at the experimental level. Ultrasonic energy
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provided easy efficient route for dye extraction, mordanting, and dyeing processes in
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comparison with the traditional methods (Mansour and Heffernan, 2011).
Kamel et al. (2005, 2007, 2009a, 2009b) comparatively investigated various parameters for
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dyeing of wool and cotton using ultrasound as well as conventional heating method and
reported that ultrasonic power substantially enhanced both dye (lac, cochineal and saffron)
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ultrasonic cavitation effect. Vankar and co-workers discussed the effectiveness of ultrasound
technology for dyeing of different type of textile fibres with commercially available natural
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dyes such as catechu, tectona (Vankar and Shanker, 2008), madder (Vankar et al., 2008d) and
identification, extraction and application of natural dyes from new vegetable sources such as
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Ixora coccinea (Vankar and Shanker, 2006), Eclipta alba (Vankar et al., 2007a), Symplocos
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(Vankar et al.,2008c), Delonix regia (Vankar and Shanker, 2009), Daphne papyraceae
(Vankar et al., 2009a), Melastoma malabathricum (Vankar et al., 2009b). Results obtained by
them in a series of experiments have shown superiority of sonicator dyeing over conventional
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dyes and electrolytes in dyeing-bath and effluent along with significant increase in dyeing
performance and color characteristics of dyed fabrics without ignoring the stability conditions
of dye molecule. Xinsheng et al. (2008) reported the merits of ultrasonic extraction of dye
from Sargentodoxa cuneata and its application on wool fabric. The use of ultrasonic energy
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in dyeing woollen fabric in presence of glucose/hydrogen peroxide based redox system in
combination with alum mordant (Mansour, 2010) and silk fabric using mild mordants
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(Mansour and Heffernan, 2011) is found to have a significant improvement in dye uptake
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representing sonication efficiency in textile dyeing. Sivakumar et al. (2009, 2011) studied
extraction of colorants from some dye yielding plants such as beet roots, Green wattle barks,
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Marigold flowers, Pomegranate rinds, 4O clock plant flowers and Cocks comb flowers and
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reported significant improvement in extraction efficiency of the colorants due to the use of
ultrasound. Guesmi et al. (2013) reported substantial improvement of about 49.62% more dye
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uptake in case of sonicator dyeing of modified acrylic fabrics with indicaxanthin natural dye
in addition to better light, washing and water fastness results than the conventional method.
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The use of ultrasonics in natural textile dyeing provides the following benefits:
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Improves processing efficiency and yield better product quality by allowing real-time
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Use of sonication method for textile dyeing on commercial scale is definitely a cleaner
method. As a general conclusion it could be said that replacing conventional thermal dyeing
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method with sonication method could make the process highly efficient, energy saving,
Recent developments in natural textile dyeing mainly rely on the modification of natural and
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synthetic fibres using various pre- and post-treatment agents for improvement in color,
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fastness and functional characteristics of dyed fabrics along with the focus on environmental
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containing cationic (Kim et al., 2004; Kim and Park, 2007) and anionic groups (Kamel et al.,
2009a, 2011; Bulut and Akar, 2012) on dyeing properties of fabrics with different types of
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natural dyes have been evaluated frequently. Results indicated that pre-treatment of different
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types of fabrics with cationic and anionic agents enhances color strength and fastness
enhancing absorption capacity naturally dyed fibers (Janhom et al., 2004, 2006). In recent
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years, a number of investigations have been carried out to exploit potential applicability of
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chitosan, a naturally occurring biopolymer with distinct chemical and biological properties,
cotton (Kavitha et al., 2007; Kim, 2006) and wool fabrics (Dev et al., 2009). The pre-
treatment of fabrics with chitosan increased the binding sites for the dyes resulting in better
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Recently, dry modification processes such as sputtering and low temperature plasma (LPT)
treatment techniques that generate no waste have been introduced for the pretreatment and
(Ghoranneviss et al., 2011; Shahidi and Ghoranneviss; 2011). Plasma treatment of fibers
improves surface characteristics of fibers while the bulk properties of the fibers are not
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affected (Barani and Maleki, 2011). Wakida et al. (1998) marked the associated benefits of
oxygen, carbon tetrafluoride, and ammonia low temperature plasma treatments of wool and
nylon 6 fabrics for dyeing with several natural dyes, such as cochineal, Chinese cork tree,
madder, and gromwell. Park et al. (2008) subjected PET fabrics to chitosan and/or O2 low-
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temperature plasma as a pre-mordant in which the fabric was processed by padding, plasma-
etching, and immersion procedure and dyed with natural dye of Caesalpinia sappan. They
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showed that pre-treatment of PET fabrics with chitosan and/or plasma is better than a metal
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mordant in terms of the dye uptake and reduction in dyeing time. Surface pre-activation using
air atmospheric plasma and ultraviolet excimer treatment have also been used to activate PET
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fibrous surfaces yielding hydrophilic species, thereby increasing dyeing affinity with
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curcumin natural dye (Kerkeni et al., 2012). Chemical modification of cotton fabric with
The inherent poor light fastness of several natural dyes is a property which limits their use in
modern day applications. The use of UV absorbers and antioxidants are reported to have
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positive effect on the light fastness of naturally dyed fabrics (Cristea and Vilarem, 2006; Lee
et al., 2001). Introduction of a singlet oxygen quenching group into an ultraviolet absorber
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prepared as a means of improving the light fastness of naturally dyed fabrics provide a novel
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approach for improving the photostability of natural dyes (Oda, 2012a, 2012b). The
photostability of an anionic natural dye can be improved by intercalation into the hydrotalcite
layer, if the dye has a hydrophilic nature and a rather planar structure. The intercalated dye is
stabilized by the protection from the attack of the atmospheric oxygen (Kohno et al., 2009).
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Hydrophobic acrylic fibers pose a big problem for dyers due to their hydrophobic nature.
hydrochloride is reported to increase substantively of the fiber towards some anionic natural
dyes (Guesmi et al., 2012a, 2013). Modified acrylic fiber containing different amounts of
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amidoxime groups showed better dye uptake along with significant improvement in color
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researchers implied ammonia after treatment as useful technique to obtain better shades with
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improved colorimetric properties (Montazer et al., 2004; Montazer and Parvinzadeh 2004).
The preliminary studies on natural dyesurfactant interactions have shown that dyeing of
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fibres with the natural dyes in the presence of the surfactants enables good shade and fastness
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in color at low temperatures to be achieved and may minimize the damage to fibres during
dyeings (Chandravanshi and Upadhyay, 2012). Use of high energy radiations such as UV
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(Adeel et al., 2012; Iqbal et al., 2008) and gamma radiation (Bhatti et al., 2010; MGarrech
and Ncib, 2009; Naz et al., 2011) had also been reported to be beneficial in improving the dye
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Pretreatment and finishing of textile fabrics by modern surface modification techniques, such
environmentally clean textile processing methodology and are much superior to traditional
sustaining green chemistry aspects of processing and application shows that there is a
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significant potential to reduce the ecological impact of existing processes with the
introduction of these new concepts in real time methodologies of textile dyeing and finishing
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In recent years, both researchers and practitioners have devoted attention to environmental
and socio-economic sustainability issues in the textile industry (Thiry et al., 2011; Caniato,
2012). Despite the industrial relevance of the issue, structured analysis of the perspectives
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relevant to socio-economic and environmental impacts is severely missing in the literature
available on natural dyes. It is one of the biggest impeding factors in industrial utilization of
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natural dyes in modern textile industry. Since natural dyeing does not exist on a commercial
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scale in modern textile industry, currently most of the studies are based on laboratory results
or model processes. However, some discrete group of researchers have investigated the
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ecological position, future demands and availability of raw material, the handling, products
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properties, renewability and standardization for large scale production of natural dyes,
leveraging on environmental and economic sustainability to reach out to new market niches
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(Bechtold et al., 2003; Bechtold and Mahmud-Ali, 2008).
Most of these studies available on natural dye sources and dyestuff extraction centered on
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collecting plant materials from wild and exploring the coloring properties of extracts from
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different plant parts. However, direct commercial use of native plants in dyestuff production
without investigating sustainability issues seems impractical and will lead to overexploitation
consequences critical to harvesting natural dye yielding crops are rare. Indigo, madder, and
weld are some well screened natural dye crops which can be profitably harvested for
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industrial application (Gilbert and Cooke, 2001). There is need for economic valuation and
environmental monitoring studies that explicitly focus on potential natural dye crops that are
not commercialized, but rather harvested and consumed directly by indigenous households
(MacFoy, 2004; Dogan, 2003; Siva, 2007). Standerdized collection of this type of
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information from local inhabitants of different parts of world on indigenous natural dye
sources that can be harvested in that particular climatic condition is a first step in assuring
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environmental and socio-economic reality. Furthermore, for the commercial exploitation, the
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selected species must also be screened for their appropriateness in purview of modern
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It is well know that the industrial system is very wasteful of materials and recycles very little
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(Ayres, 2004). Industrial sectors are experiencing the challenges of building up new systems
which have the capacity to recycle or reuse theses waste materials at minimal cost leading to
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the fulfillment of economic development and environmental sustainability objectives. The
idea of zero emission based on the notion that every biological waste is food for some other
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organism leads to the idea that some industry can always be found to consume another
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industrys wastes, although not always true, is very reasonable in natural dye production
from industrial wastes. Use of cheap by products from agriculture and forestry such as bark
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from timber industry e.g. Ash tree bark (Bechtold et al., 2007a), and leaves from abundantly
available palnts such as teak (Prusty et al., 2010), eucalyptus (Mongkholrattanasit, 2010), is
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a promising concept which can lower costs involved in natural dye production. Industrial
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food and beverage production produces huge amount of coloured plant wastes such as
pressed berries and distillation residues (Bechtold et al., 2006), pomace (Bechtold, 2007b),
peels (Sinha et al., 2012), shell (Ismal and Yildirim, 2012), and other residual by products
(Meksii et al., 2012) containing considerable quanitities of coloring matters which can be
utilized as promising source of natural dyes for textile industries after some careful
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investigation of supply chain system and optimization of processing variables (Bechtold and
Mahmud-Ali, 2008; Bechtold et al., 2009). Olive mill wastewater (OMW), (a by product of
countries, as around 30 million m3 of OMW produced annually in this region) can be used as
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prospective source of natural coloring substances in olive oil producing countries which are
renewable, available in high quanitities and free costs (Meksi et al., 2012). An intensified use
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of industrial waste as renewable raw material for natural dye production represent
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sustainable cleaner production strategy as in addition to minimizing waste production and
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Production cost of natural dyes from direct harvesting are high as compared to production
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costs from waste and by-products. However, colours provided by agricultural primary
production could not be obtained with residues. Thus, any industrial natural dye production
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unit must include both direct agricultural as well as residual sources for obtaining a complete
color pallete. Strategic combination of different plant sources allows the minimization of
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cost to certain extent, and the average production cost of total color portfolio could be within
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the range of synthetic colorants (Geissler, 2009). Thrusting on minimizing the chemical load
of extraction procedure, Bechtold and coworkers suggested explicit use of water solvent in
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extraction of natural dyes from different sources (Bechtold et al., 2003, 2006; Bechtold and
Mahmud-Ali 2008). The use of other solvents may lead to highly contaminated waste water
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and plant residue, which require complicated aftertreatments leading to additional costs from
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solvent and chemical consumption and expensive deposition of contaminated wastes. They
also suggested combined dyestuff extraction and subsequent dyeing, as it will reduce
transportation cost and energy requirements of the process. Low exhaustion rates of natural
dyeing process is of great concern: firstly, it increases cost of dyeing process as unfixed dye
is not available for the coloration process and secondly, the dye present in the wastewater
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has to be removed in order to fulfill legal limits for textile effluents (Mussak and Bechtold,
2009).
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greater extent thus decrease the effleuent load and cost of natural dyeing (Sivakumar et al.,
2009; Mansour and Heffernan, 2011). Research findings on using enzyme as fabric pre-
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treatment method offers a cost effective and environmentally favorable soft chemistry
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option as enzymes are specific and fast in action and small amounts of enzyme often save
large amounts of raw materials, chemicals, energy and water (Vankar and Shanker, 2008;
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Montazer et al., 2009). Another interesting aspect is reusing spent dye liquor in repeated
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dyeing cycles (Vankar et al., 2007b). Economic analysis as done by Shams-Nateri (2011) on
reusing waste water for wool dyeing with madder caused 19.91% cost saving.
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Huge amount of biomaterials are required for large scale production of natural dyes. Because
of low dye content of natural dye yielding plants, large amount of waste generated after
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natural dye extraction creates an additional burden of waste disposal. Vankar et al. (2011)
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presented a very interesting study on biosorption efficacy of waste pulp generated after
natural dye extraction from some selected biomaterials (Canna indica flower, Portulaca
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olecera flower and stem, Hibiscus rosa sinensis flower and Trapa natans fruit skin) as an
alternative use other than just composting it. The demaonstrated that use of natural dye waste
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as heavy metal adsorbents can be very effective in remediation of groundwater and surface
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It is undeniable that natural dyes are only used in a small scale by craftspersons, hobbyist
and indigenous people, and hardly used in modern textile industry. However, the emerging
body of literature on the environmental and economic issues of natural textile dyeing
demonstrates that, as the environmental impact is reduced throughout the whole life cycle
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(Fig. 2), the use of natural colorants is expected to contribute to sustainable development in
The role of the textile finisher has become increasingly demanding, and now requires a
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careful balance between compatibility of different finishing products and treatments and the
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application processes used to provide textiles with desirable properties. Consumers
worldwide are looking for clothing and other textile products which provide greater comfort
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and remain fresh, hygienic and odor free in use. Investigation for innovative methods, for
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applications and problems in this area is the need of the hour. A number of reports are now
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available on natural colorants for imparting multifunctional properties to textiles such as
antimicrobial (Singh et al., 2005), insect repellent (Kato et al., 2004), deodorizing (Hwang et
M
al., 2008; Lee et al., 2008) and UV protective (Sarkar, 2004) properties. Chemical
constituents of some important natural dyes used in functional finishing of textiles are given
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in Fig. 3.
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Textiles have long been recognized as a media to support the growth of microbes as they
provide excellent environment for microbial growth and proliferation. Microbial growth on
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textiles during use and storage imposes a number of undesirable effects for the textiles as
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well as users. These effects include generation of foul odors, discoloration, mildew
formation, apparel degradation, dermal infection, allergic responses and other related
diseases. A variety of synthetic antimicrobial textile agents have been reported such as
chitosan, polybiguanides, triclosan, nanoparticles of noble metals and metal oxides, and
bioactive plant-based products (Gao and Cranston, 2008; Simoncic and Tomsic, 2010). Most
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of them are complex in nature and take long time to complete their natural cycles and return
to nature. The challenges faced by textile finishing industry have intensified because of the
potential environmental risks and health and safety concerns emerging from use of synthetic
antimicrobial agents. There has been a growing need to develop eco-safe functional finishing
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agents for making textile products that can offer improved protection to the users from
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used in wide range of clothing, home furnishings, commercial and industrial products (Gupta
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and Bhaumik, 2007; Ramchandran et al., 2004). With the steady increase in number of safe
and durable antimicrobial agents and textile finishing techniques, bioactive textiles are easily
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finding a place in the global textile market. Recent developments in bioactive agents of
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natural origin have opened new avenues in this area of research (Joshi et al., 2009).
Therapeutic properties of a number of dye yielding plants is well know and some of these
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have been shown to posses significant antimicrobial effect (Calis et al., 2009; Gupta et al.,
2005; Lee et al, 2009). The antimicrobial activity of some of these dyes is reported as potent
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owing to the existence of tannins (Prabhu and Teli, 2011; Shahid et al., 2012), flavonoids
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(Cushnie and Lamb, 2005), curcuminoids (Han and Yang, 2005), alkaloids (Kim and Son,
2005), and quinones (Khan et al., 2012) in their extracts. During last few decades, many non-
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toxic natural products have been tested for antimicrobial activity after application on wool,
cotton and other textile material with good results (Joshi et al., 2009).
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Gupta and co-workers have studied antimicrobial properties of eleven commercially available
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natural dyes against some pathogenic gram positive and gram negative bacteria (Gupta et al.,
2004, 2005; Gupta and Laha, 2007; Singh et al., 2005). Antimicrobial activities of these dyes
are dependent on chemical structure and functional groups present in dye molecules. The
authors reported that tannin based natural dyes were most effective in inhibiting microbial
growth. They also ascertained that antimicrobial activity of a dye would vary when it is
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present in solution form than when it is held intimately to the textile substrate. Han and Yang
class) after application on wool fabrics and established a quantitative relation between the
inhibition rate, curcumin concentrations and K/S values of treated woollen fabrics. Based on
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these relations, antimicrobial activity of wool fabrics finished with curcumin can be predicted
on the strains of S. aureus and E. coli without antimicrobial testing. Berberine, a natural
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cationic colorant was successfully employed onto cotton (Kim and Son, 2005), wool (Ke et
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al., 2006) and nylon (Son et al., 2007) to produce yellow colored fabrics with excellent
antimicrobial activity. Ammayappan and Moses (2009) used Aloe-vera, chitosan and
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curcumin each separately as well as in different combinations to impart antimicrobial activity
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to cotton, wool and rabbit hair substrates. They revealed that peroxide treated cotton and
formic acid treated wool/rabbit hair substrates shows better antimicrobial activity than
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corresponding intact ones. Antimicrobial tests conducted on natural dyes obtained from
different plant waste materials such as waste leaves and superficial barks of Terminalia
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catappa, Artocarpus heterophyllus, Tectona grandis, Morinda citrifolia (Prusty et al., 2010),
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Albizia lebbek and Saraca asoca (Baliarsingh et al., 2012) demonstrate an exciting
opportunity for producing naturally dyed silk yarn as a potential sustainable technique
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towards waste utilization and development of protective clothing. Ibrahim et al. (2010)
investigated various factors affecting dyeing and multifunctional properties of knitted cotton
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fabric such as fabric structure, type and concentration of mordants, kind and percent of
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natural dye extract and dyeing procedure. They reported that susceptibility of tested microbes
to killing as they contact the surface of dyed samples are in order as G+ve > G-ve; most
probably due to the fact that G+ve bacterial cell wall consists of a single layer whereas G-ve
cell wall is multilayered bounded by outer cell membrane. Reports on effect of different
metallic salt mordants on antibacterial and antifungal activity of woollen yarns dyed with
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Acacia catechu (Khan et al., 2011), Lawsonia inermis (Yusuf et al., 2011, 2012), Rheum
emodi (Khan et al., 2012) and Quercus infectoria (Shahid et al., 2012) extracts showed that
mordanting with metallic salts decreased the antimicrobial activity of dyed yarns to some
extent, however durability of antimicrobial activity increased manifold. This could be the
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consequence of complex forming ability of metal salts with active functional groups of dye.
Some pigment producing fungi are also reported as potent sources of natural colorants which
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can be applied as antimicrobial finishing agents on silk (Saranya et al. 2012), cotton and
SC
leather (Velmurugan et al., 2009). Use of biomordants in place of metallic salt mordants is
found quiet helpful in enhancing antimicrobial activity of naturally dyed textile fabrics
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(Prabhu et al., 2011, Prabhu and Teli, 2011). Few recent reports pointed out the use of
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modern innovative methods such plasma treatment (Chen and Chang, 2007; Ghoranneviss et
al., 2011), chitosan treatment (Dev et al., 2009), enzymatic treatment (Raja and Thilagavathi,
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2011), cationization (Hong et al., 2012), microencapsulation and cross-linking
naturally dyed textile materials. These innovative methods proved of immense help in
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Although, several efforts have been made to exploit various natural dyes for antimicrobial
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finishing of textiles, but still there is scarcity of systematic and logical approach for
implementation of these findings in real market of protective antimicrobial textiles. There are
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several key issues which are still remaining to be looked into. The major challenge in
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application methods as the activity and composition of natural dyes obtained from same
source varies depending on their geographical location, method of extraction and application.
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Durability of finishing is a major concern to textile researcher and users since the finished
products are subjected to frequent laundering. Emphasis should be paid on the durability of
the treatment during conditions of subsequent storage and use, such as the rubbing, washing
and light exposure. The findings reported in cited literature demonstrate an exciting
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opportunity for the naturally dyed textile as a potential perspective in developing protective
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3.2. UV-protective finishing
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Ultraviolet radiation (UVR) from the sun causes sunburns, tanning, premature skin aging and
wrinkling and its overexposure leads to skin cancer (Narayanan et al., 2010). Lifestyle
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changes such as excessive exposure to sunlight during leisure activities have increase chances
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of skin cancer. Exposure to the sun is an occupational hazard to outdoor workers such as
properties of textiles are influence by many factors such as structure and physiochemical
nature of fibre, dyes and finishes, fabric thickness, porosity and moisture content (Gies, 2007;
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Sarkar, 2007). Fabric color also has a fundamental importance in UV protection (Grifoni et
al., 2009). The sun rays blocking properties of a textile are enhanced when a dye, pigment,
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delustrants, or ultraviolet absorber finish is present that absorbs ultraviolet radiation and
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blocks its transmission through a fabric to the skin; thus dyed fabrics protect more than
undyed ones and their protection levels rise with the increase in dye concentration (Hustvedt
Sarkar (2004) characterized Ultraviolet Protection Factor (UPF) of plain, twill or sateen
weave cotton fabrics dyed with colorants of plant (madder and indigo) and insect (cochineal)
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origins with respect to fabric construction, weight, thickness and thread count. A positive
correlation exists between the weight, thickness and shade depth of the naturally dyed fabric
and their UPF values; however thread count appears to negatively correlate with UPF.
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natural dyes (Rheum and Lithospermum erythrorhizon) applied on cotton and silk found that
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Results demonstrated that UV-protective effect was strongly dependent on absorption
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characteristics of natural dyes for UVR. Grifoni et al. (2009, 2011) studied the effect of color
on UVR transmission of cotton, flax, hemp and ramie fabrics with different construction
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parameters dyed with some common natural dyes by in vitro and outdoor assessments. The
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comparison between two methods applied to measure fabric transmittance pointed out that
the UPFs calculated by in vitro measurements were generally lower than those based on
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outdoor data, indicating an underestimation of actual protection level of tested fabrics
assessed by in vitro test. Metallic salt mordants have been reported to enhance UV-protective
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properties of naturally dyed cotton (Gupta et al., 2005), wool (Mongkholrattanasit et al.,
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2011a) and silk (Mongkholrattanasit et al., 2011b; Wang et al., 2009) fabrics to a substantial
account depending on nature of fibre, mordant and natural dye used. Very recently, Hou et al.
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(2013) used natural dyes extracted from orange peel (OP), an abundant, cheap and readily
available agricultural byproduct, for producing highly durable UV protective wool fabrics.
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They reported that UPF value of OP treated wool fabric was six times higher than that of the
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wool fabric dyed with normal synthetic dyes with similar shade and depth of shade and even
after 30 home laundering cycles, the UPF value of the OP dyed wool was found 4 times
To avoid the health risks associated with UV exposure, the use of sunscreens and UV
protective clothing has gained popularity among masses. Textiles have been considered
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exhibit enormous differences between fabrics due mainly to their structure, composition and
color. Textile industries see a promising future for UV protective fabrics, with the
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for the world market. Therefore, it is contemporary need to develop a proper treatment to
increase the UV protection property to fabrics. Promising research findings obtained from
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laboratory scale and outdoor experiments shows that naturally dyed fabrics with UV
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protective properties seem to have bright future after some rigorous research and
development.
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3.3. Insect repellent finishing
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Insect damage on textile products such as carpets, garments, upholstered furniture, blankets,
and priceless heirlooms is a serious problem faced during storage and results in significant
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economic losses, especially in warehouses and showrooms. Even a small amount of fibre
eaten from a valuable suit or a rug can ruin its functional and/or aesthetic properties. Insect
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repellents that discourage insect damage in textile industry are in great demand. Kato et al.
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(2004) studied damage to wool fabrics dyed with ten different natural dyestuffs by the larvae
of varied carpet beetle, Anthrenus verbasci. Eight among the ten natural dyestuffs were found
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effective against A. verbasci and strength of their repellent effect in feeding preference test
was in the order of lac dye, gallnut, catechu, red cabbage, Cricula cocoon extract > cochineal,
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indigo, Amur cork tree extract. Park et al. (2005) studied in detail the insect resistance of
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eight naturally occurring quinones and flavonoid dyes after application to wool with five
mordanting agents by using laboratory-reared black carpet beetles. The anthraquinone dyes,
such as cochineal and madder, were found to be very effective in protecting wool fabric
against black carpet beetles. Madder resulted in lowest weight loss and the best effect of
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At present, we are mostly dependant on fossil fuels i.e. coal, crude oil and natural gas for our
energy needs. These fuels being non-renewable and limited in supply are constantly
exhausted, thus are creating a huge problem for the future generations. Therefore, a search for
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renewable low environmental impact alternative energy sources is considered one of the top
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priorities in today's society. Among renewable energy resources, solar energy is the largest
exploitable resource, which provides more energy in 1 hour to the earth than all of the energy
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consumed on the planet in one year (Lewis and Nocera, 2006).
A dye-sensitized solar cell (DSSC) (Fig. 4) is a third generation photovoltaic device for the
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conversion of visible light into electric energy which provides a technically and economically
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credible alternative concept to present day pn junction photovoltaic devices (Gratzel, 2003).
It has emerged as one of the promising renewable energy sources for eco-friendly and cost
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effective conversion of solar energy to electricity and due to the use of inexpensive materials,
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simple fabrication process and low environmental impact, especially those sensitized by
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natural dyes (Narayan, 2012; Patrocinio et al 2009). Dye-sensitized solar cells are innovative
solar cells that mimic photosynthesis in plants. Unlike traditional solar cells, dye-sensitized
EP
cells can work effectively in low light conditions and are less susceptible to losing energy to
heat. The efficiency of DSSC is determined mainly by the sensitizer used. The dye as a
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sensitizer plays a key role in absorbing sunlight and transforming solar energy into electrical
AC
energy (Zhou et al., 2011). DSSCs with efficiencies of up to 11% have been designed using
ruthenium (Ru) based dyes but the limited availability and high cost of these dyes together
with their undesirable environmental impact have led to the search for cheaper and safer dyes
There have been some interesting explorations of natural dyes in the context of the dye-
sensitized solar cell (DSSC) application using pigments obtained from biomaterials. Several
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reports have emphasized on exploration into natural dyes, such as cyanine (Sirimanne, 2006),
anthocyanins (Fernando and Senadeera 2008; Zhu et al, 2008), cyanidins (Senthil et al.,
2011), tannins (Espinosa et al., 2005), chlorophyll and their derivatives (Chang and Lo, 2010;
Calogero et al., 2009), carotenoids (Yamazaki et al, 2007), betalains (Calogero et al., 2012;
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Zhang et al., 2008), chalcones (Agarkar et al., 2011), and many others (Ito et al., 2010; Sang-
aroon et al., 2012) as a cheaper, faster, low-energy requiring and environment friendly
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alternative for use in dye sensitized solar cells. Although these natural dyes often work
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poorly in DSSCs, these are expected as low cost and prepared easily comparing to ruthenium
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Different types of natural dyes showed different solar conversion efficiencies depending on
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the source and chemical structure of dye and interaction between dye molecule and photo
electrode i.e., TiO2, ZnO etc (Hao et al., 2006; Narayan, 2012; Thambidurai 2011; Zhou et
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al., 2011). Natural dye sensitized DSSCs usually perform poorly in DSSC because of weak
binding energy with the metal oxide film (photo-electrode) and low charge-transfer
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absorption in the whole visible range. Based on investigation on the structure and properties
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of dye molecules, the best photosensitized effect in the some of the tested natural dyes is
obtained due to the better interaction between the different binding groups of dye molecule
EP
on and the TiO2 film on cathode in DSSCs. Heera and Cindrella (2010) theoretically
evaluated ten natural pigments: caffeic acid, ferulic acid, ellagic acid, deoxysantalin,
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resveratrol (plant source), carminic acid, kersemic acid, ommatin D (insects), methoxatin and
AC
caulerpinic acid (microbes), as photosensitizers for their possible application in DSSC and
concluded that resveratrol, ferulic acid, caffeic acid and methoxatin can prove potential
pigments for efficient application in DSSC due to their favourable wavelength maximum
much compatible with TiO2 and their high oscillator strength. Gomez-Ortiz et al. (2010)
investigated the use of bixin and norbixin obtained from achiotes seeds in DSSCs based on
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TiO2 and ZnO substrates and confirmed that the efficiencies obtained with TiO2 are much
higher than for ZnO substrates, in agreement with the general trends observed for these two
substrate materials. Yamazaki et al. (2007) assembled DSSCs by using natural carotenoids,
crocetin and crocin, as sensitizers and demonstrated that, crocetin can attach effectively to the
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surface of TiO2 film due to the presence of carboxylic groups in the molecule and perform the
better photosensitization effect than crocin that has no carboxylic group in the molecule.
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Extracting temperature, extracting solvent and pH of the extract solution also have very
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prominent role in determining efficiency and stability of DSSCs (Chang et al., 2010;
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Meng et al. (2008) elucidated the electronic coupling between a TiO2 nanowire and a
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cyanidin natural dye sensitizer and provided insight into charge injection mechanisms of
natural-dye sensitized nanowire solar cells. By exploring various nanowire orientations and
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dye adsorption sites they showed that their system has additional advantages over traditional
DSSCs such as free availability of the dye, large surface area, environmentally benign
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components, and improved light scattering and charge transport, all of which contribute
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toward improving key characteristics, that is, low cost and high efficiency. DFT
sensitized solar cells for better understanding of the electron injection process is also reported
Several innovative methods have been developed for performance improvement of natural
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natural dye anthocyanin-sensitized solar cells can potentially improve the mechanical and
al., 2008). In another experiment overall conversion efficiencies of DSSCs fabricated with
natural sensitizers obtained from pomegranate juice for cells operated with Pt
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electrodeposited counter electrode were found much higher than carbon coated counter
electrode (Bazargan, 2010). Luo et al. (2009) assembled DSSCs by using electrophoresis
technique for fabrication of TiO2 film with natural dyes extracted from C. indica L., S.
splendens, cowberry and S. nigrum L. as sensitizers. Dai and Rabani (2001; 2002) employed
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anthocyanins extracted from pomegranate as aqueous mediators for DSSCs and studied the
effect of the mediator solvent in the performance of solar cells sensitized by commercially
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available anthocyanins. Sandquist and McHale (2011) explored the use of a blocking layer
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and treatment by TiCl4 in order to optimize the performance of the betanin-based dye-
sensitized solar cells, and recorded the highest energy conversion efficiencies as high as 2.7%
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for a DSSC containing a single unmodified natural dye sensitizer. In a combined
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experimental and theoretical study of natural betalain pigments Oprea et al. (2012) identified
betacyanins as the useful constituents of red beet root extract as natural sensitizers and
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emphasized on the role of extract purification for better results. Kumara et al., (2006)
from shiso leaves and successfully achieved broadening of spectral response of dye sensitized
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solar devices. Synergistic effect of mixed pigments in the energy transfer of the pigment
sensitized mesoporous TiO2 solar cells was further confirmed by experiments on DSSCs
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fabricated with mixed chlorophyll and xanthophylls pigments extracted from different plants
(Bao-Qi et al., 2008). Eenergy conversion efficiencies and maximum power output for solar
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cells sensitized by mixed pigments were much higher than that achieved by the linear
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various DSSCs using natural dyes of red cabbage, curcumin, red-perilla and their mixtures.
They found that the conversion efficiency of the solar cells fabricated using the mixture of
red cabbage and curcumin was much larger than that of solar cells using one kind of dye.
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They also reported that the cost performance of solar cells sensitized with red cabbage is
lower by more than 50 times than that of solar cells using Ruthenium complexes.
In a recent study, Park et al. (2013) observed that procedure of adsorbing the binary dye onto
TiO2 film is also a very important factor in determining the performance of fabricated cells.
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They reported that the energy conversion efficiency of the TiO2 electrode with successive
adsorptions of gardenia yellow (GY) and gardenia blue (GB) dyes was 0.59%, which is
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enhanced compared to single dye adsorption (0.32% for GY and 0.16% for GB), however
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adsorption of GY and GB dye mixture resulted in much lower energy conversion efficiency
(0.04%). The decrease in efficiency of such cocktail dyes due to unfavorable interactions
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between the two dyes.
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Incorporation of a natural dye sensitized solar cell fabrication module in conventional science
Graztel, 1998). Few researchers have taken into account the educational importance of
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renewable energy resources (Calogero and Marco, 2008; Raturi and Fepuleai, 2010; Smestad
1998).
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Despite the effort involved the in use of natural dyes as sensitizers, low conversion
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Although a number of natural dyes have been tested for their performance in DSSCs (Table
4), most of them yielded conversion efficiencies of less than 1%. Betanin extracted from beet
roots, =2.71% (Sandquist and McHale, 2011), Xanthomonascin-A extracted from Monacus
purpureus, =2.3% (Ito et al., 2010), and isobutrin from Butea monosperma, =1.8%
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(Agarkar et al., 2011) were found to be the best photosensitizers for use in DSSCs compared
with other natural dyes, except for some chlorophyll derivatives which yielded conversion
exhibited energy conversion efficiencies over 4% (Ikegami et al., 2008). The efficiency of
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natural dye sensitized solar cells is determined by a number of factors that include selection
of the appropriate natural dye, quantitatively significant stable electronic anchorage of the
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dye to the surface of the metal oxide nanostructure, choice of photoanode, counter electrodes,
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electrolyte and solvent system. It is therefore highly desirable to standardize these critical
factors in the context of making natural dye sensitized solar cells a commercially viable
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option. The advantages of natural dyes as photosensitizers are large absorption coefficients,
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high light-harvesting efficiency, no resource limitations, low cost, simple preparation
techniques and no harm to the environment. Although the efficiencies obtained with these
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natural dyes are still below the current requirements for large scale practical applications,
these interesting explorations of fabrication of dye-sensitized solar cell using dyes obtained
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from bioresources invoked participation of researchers around the globe to engage in research
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to search for new sources of natural dye systems that are stable, nontoxic, biocompatible and
have desirable optoelectronic properties. Some serious efforts in natural dye sensitizers may
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As a consequence of growing worldwide concern for food quality and safety, a set of
standards have been brought in by different governments. Market pressure brought about by
changes in legislation and consumer preferences have necessitated the foods to be formulated
with more natural ingredients. The use of natural pigments for food coloring is receiving
growing interest from both food manufacturers as well as consumers and there has been much
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interest in development of new natural colorants for use in food industry in the continuing
replacement of synthetic food dyes because natural products are associated with quality and
health promotion whereas synthetic pigments are critically assessed by consumers (Dawson,
2008; Downham and Collins, 2000; Henry, 2000). Standardized methods of collection,
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extraction, purification, stabilization and standardization for a variety of natural food
colorants are available such as anthocyanins (Wrolstad, 2004), betalains (Azeredo, 2009; Roy
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et al., 2004; Stintzing and Carle, 2007), chlorophylls (Humphrey, 2004; Kong et al., 2012),
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carotenoids (Mortensen, 2006), tannins (Vankar et al., 2006), Monascus (Dufosse et al.,
2005), quinones (Gonzalez, 2002), biliproteins (Sekar and Chandramohan, 2008), safflower
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(Cho et al., 2000), turmeric (Marcolino et al., 2011) etc. They have different groups of
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chemical compounds which may be used directly as colorants or in chemically modified form
to produce different hues ranging from green through yellow, orange, red, blue, and violet,
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depending on the source of colorant or increased stability (Bakowska-Barczak, 2005).
Researchers willing to experiment and expand this interesting palette of natural food color
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In most of the countries strict regulations have been formulated regarding the use of food
additives including colorants. Perhaps, every country has its own basic color additive
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regulations, and acceptable standards vary widely from one country to the other. With
dwindling number of approved synthetic colors over the years, researchers have devoted
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more attention to the development of natural food colors, as they are generally more
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internationally accepted (Burrows, 2009). Table 5 lists naturally derived colorants approved
by EU, USA and Japan for use in food coloring. Downham & Collins (2000) portrayed a very
technologies for food colorants by taking backdrop of recent developments. They concluded
that the natural food color market will grow on a global scale at a faster rate than synthetic
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colors owing to a continued consumer pressure to `go natural'. The production of many
dependence on supply of raw materials and variation in extracted pigments (Mapari et al.,
2005). A number of reports are available on exploitation of the potential of new sources of
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plants (Castellar et al., 2008; Longo and Vasapollo, 2005; Lin et al., 2010) and insect
(Gonzalez, 2002; Borges et al., 2012) origin as well as other biological sources such as fungi
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(Duran et al, 2002; Mapari et al, 2005; Velmurugan et al., 2010), bacteria (Zhang et al.,
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2006), and algae (Campo et al., 2007; Dufosse et al., 2005) in addition to those covered by
existing legislations. Most of the currently used natural pigments are highly sensitive to pH
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change, temperature and prone to light, heat and oxygen disintegration (Delgado-Vargas et
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al., 2000). Ascertaining the color stability of natural colorants as pre-requisite for their
2006). Although, the wealth of information is now available on new sources for food
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colorants, however, any new pigment source would require rigorous assessment of
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established safety tolerances and should meet the economic, legal and aesthetic requirements,
Pigments producing microbes such as fungi, bacteria and microalgae are quite common in
nature. Among the molecules produced are carotenoids, melanins, flavins, quinones and more
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has been seen in recent times in biotechnological production of food grade pigments
(Chattopadhyay et al., 2008). A number of alternative biosynthetic methods are available for
the commercial production of natural colors using diverse microbial sources. With recent
advances in genetic engineering technology, attempts have been made to create microbial cell
factories for the production of food colorants through the heterologous expression of
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biosynthetic pathways from either already known or novel pigment producers (Dawson,
2009). The use of fungi to color foodstuffs is not new; Monascus pigments are being
traditionally used in food in the Orient for hundreds of years. Fungi provide a readily
available alternative source of naturally derived food colorants. The recent approval of a
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fungal food colorant has tremendously increased the prospects of research to explore the
extraordinary chemical diversity and biodiversity of fungi for the biotechnological production
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of pigments as natural food colorants. Recent data indicate that with an appropriate selection
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of suitable fungus using chemotaxonomic tools and a priori knowledge of fungal extrolites,
fungi can be used as cell factories for pigment production and could be developed to tailor
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functionality and expand the color palette of existing natural food colorants; the fungal
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natural colorants could be produced in high yields by using the available cultivation
technology without potential genetic manipulation since tougher legislation and skeptical
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attitude of consumers make it rather difficult for the acceptance of genetically modified food
(Mapari et al., 2005, 2006, 2009, 2010). Micro-algae are also seen as a major natural source
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for a vast variety/array of natural colors. Campo et al. (2007) presented a beautiful picture of
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cultivation. Carotenoid production has been proved to be one of the most successful branches
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of biotechnology of microalgae.
Innumerable associated benefits and myriad therapeutic properties are linked with the use of
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natural colorants in food industry (Chattopadhyay et al., 2008; Siva et al., 2011). For
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example, in addition to coloring property, anthocyanin extracts may act as quality control
marker for food stuffs; improve the nutritional quality of foods and beverages, possibly play
an important role in reducing the risk of coronary heart disease, cancer, and stroke (Wrolstad,
2004, 2005). Carotenes are also used for nutritional purposes an essential vitamin source
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vitamin C, whereas riboflavin contains vitamin B (Burrows, 2009). Many of the natural food
colorants possess excellent antioxidant properties (Beutner et al., 2001). Flavonoids and
tannins are recognized as colorants with high pharmacological value (Chattopadhyay et al.,
2008). Thus, in addition to their primary function of improving the visual quality of food
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products, naturally derived food colorants may improve the nutritional value of the target
food. These prospective nutraceutical properties may play increasingly important role in
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making a choice between natural or syathetic food colors at a time, where human diet is more
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and more based on processed foods (Stintzing and Carle, 2007).
Appearance, consumer preferences and safety standards of foods and food colors coupled
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with economics and application technology will always play a key role in the success of new
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food products. At one time, synthetic colors were the first choice as food colorants and
food coloration is resulted due to stringent regulatory pressure, bad publicity for the synthetic
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food colors and need for globally approved colorants (Frick, 2003). With biotechnological
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production of the existing colorants and find new colorant sources for their
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new ways for existing pigments and improvement of existing sources by mutation or genetic
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engineering techniques better pigments production yield could be achieved. Although many
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advances in the developments of natural food colors covering different aspects such as
well as related hygiene and safety criteria have been made over the last three decades there is
still a great scope for the discovery of relatively better and more stable natural pigments that
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In addition to above mentioned applications, there is a growing interest for using natural dyes
to dye leather (Sivakumar et al., 2009; Selvi et al., 2013); to stain wood (Goktas et al., 2008),
pulp (Savvidou and Economides, 2007), and some plastics (van den Oever, 2004); to add
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color to cosmetics (Kapoor, 2005; Kapoor et. al, 2008); to dye hair (Boonsong et al., 2012;
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Komboonchoo and Bechtold, 2009; Rao et al., 2008); to impart color to some pharmaceutical
preparations (Chigurupati, 2002); and also in histological staining (Tousson, and Al-
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Behbehani, 2011). Different prospects of natural colorants used in/as cosmetics products are
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different sources with active functional components have shown high biological activities,
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and exhibited different properties depending on each kind of pigments which makes them
excellent coloring materials for natural cosmetics and functional health foods (Boo et al.,
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2012). van den Oever et al. (2004) studied the application of several food grade colorants for
use in coloration of thermoplastics and suggested some of best performing natural colorants
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such as indigo and anthraquinone-based colorants can be used in appliances where moderate
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properties concerning heat resistance and (UV) light stability are required, such as indoor PP
applications and PVC water drainage pipes. Use of curcumin as sensitizer for
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photopolymerization of styrene is also reported (Mishra and Daswal, 2007). Siva et al. (2008)
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reported an easy, practical and reliable procedure for using Bixa orellana L. natural dye as an
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alternative tracking dye for gel electrophoresis in place of regularly used dye marker
bromophenol blue (BPB). Another very common aspect of natural dye application is their use
as pH indicator (Khan and Farooqui, 2011; Mishra et al., 2012; Ramamoorthy et al., 2009).
Shin et al., (2010) developed thermo-regulating natural indigo dyed fabrics through the
fixation of the Microcapsules (MCs) containing n-octadecane and n-eicosane on the back side
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of the fabrics using the dot-screen printing method. They obtained relatively good latent heat
storage capacity and color durability to rubbing, laundering, and ironing. Recently, Singh et
al. (2010) demonstrated the potential use of naturally derived vermillion and indigo dye in
Cheiloscopy (study of lip prints) for forensic applications. Anthocyanin based natural dyes
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are also tested as safe TiO2-sensitizer for photodergadation of organic contaminants in water
purification systems as a promising replacement for more costly and hazardous heavy metal
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based systems such as CdS particles and Ru-compounds (Zyoud et al., 2011). Kuswandi et al.
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(2012) employed curcumin natural dye as chemical sensors for detection of volatile inorganic
and organic amines produced during bacterial growth in shrimp samples. They showed that
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curcumin immobilized on bacterial cellulose membrane (biopolymers) can be used as a
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package sticker sensor for the visual detection of shrimp spoilage and could offer an extra
analytical device both to the fish industries and retailers who are interested in approaches and
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devices that are rapid, disposable, non-destructive, safe, low cost, simple, and with real time
applications. Sharma et al. (2012b) explored a new arena in the applicability of natural dyes
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isolated from R. emodi, revealing the use of dye as an extrinsic probe to determine the
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Researchers have lately explored the promise of some historical pigments such as indigo and
thin films of indigo and Tyrain purple have shown their good charge transport properties for
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use in organic electronics as natural and sustainable semiconductors. Indigo and Tyrian
purple form highly ordered thin films that afford ambipolar charge transport with relatively
high mobilities. Inspiring results have shown that these biomaterials can compete with the
best organic electronic materials and in conjunction with other biomaterials (i.e. substrate,
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electronics for many low cost applications (Gowacki et al., 2012; Irimia-Vladu et al., 2012;
Robb et al., 2013). Reddy et al. (2012) reported reversible lithium ion storage properties of a
naturally occurring and abundant organic compound purpurin, a non-toxic dye derived from
widely available plant madder, to develop sustainable and eco-friendly lithium ion
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batteries. The lithium batteries assembled using purpurin and chemically lithiated purpurin
(CPL) as working electrode showed good charge/discharge characteristics with very good
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reversible lithium ion storage properties. Future largescale application of sustainable organic
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electronics based on biodegradable materials would have a positive impact on the current
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These interesting findings on newly discovered panoramas of natural dye applications invoke
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great expectations for further research on utilization of natural dyes in a wide variety of fields
Natural dyes, generally supposed to be cheap, nontoxic, renewable and sustainable resource
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with minimal environmental impact, have attracted the attention of the scientific community
to use them in a variety of traditional and newly discovered application disciplines. Although,
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past few years have witnessed substantial growth in our understanding of technological
details required for efficient utilization of colorants obtained from natural sources, but still
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there are a number of technical challenges in each area of natural dye application that must be
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overcome before these technologies can be adopted on a practical large scale. Improving
currently challenging because of the large diversity of natural dye sources. Enthusiastic
studies discussed in the present article assert that current incompatibility of commercial
exploitation of laboratory scale results can be carried off with some serious efforts. The data
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generated from these studies may device the basis for the economic viability of natural dye
the area of natural dye applications is underway worldwide, but practical implementation to
adopt new technologies for making natural dyes a compatible co-partner with synthetic dyes
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in different spheres of our life is a long term prospect.
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Acknowledgement:
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Financial support provided by University Grant Commission, Govt. of India; through BSR
Research Fellowship in Science for Meritorious Students (Mohammad Shahid) and Research
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Fellowship to Central University Ph.D. Students (Shahid-ul-Islam) is thankfully
acknowledged.
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Refrences:
D
Adeel, S., Bhatti, I.A., Kausar, A., Osman, E., 2012. Influence of UV radiations on the
TE
extraction and dyeing of cotton fabric with Curcuma longa L. Indian J. Fibre Text. Res.
37, 87-90.
EP
Agarkar, S.A., Kulkarni, R.R., Dhas, V.V., Chinchansure, A.A., Hazra, P., Joshi, S.P., Ogale,
S.B., 2011. Isobutrin from Butea Monosperma (Flame of the Forest): A Promising New
C
Natural Sensitizer Belonging to Chalcone Class. ACS Appl. Mater. Interfaces 3, 2440
AC
2444.
Ahmed, N.S.E., El-Shishtawy, R.M., 2010. The use of new technologies in coloration of
Ali, S., Hussain, T., Nawaz, R., 2009. Optimization of alkaline extraction of natural dye from
Henna leaves and its dyeing on cotton by exhaust method. J. Clean. Prod. 17, 61-66.
38
ACCEPTED MANUSCRIPT
Ammayappan, L., Moses, J.J., 2009. Study of Antimicrobial Activity of Aloevera, Chitosan,
and Curcumin on Cotton, Wool, and Rabbit Hair. Fiber. Polym. 10, 161-166.
PT
RI
Cotton fabric dyeing with cochineal extract: influence of mordant concentration. Color.
SC
Technol. 127, 39-46.
Ayres, R.U., 2004. On the life cycle metaphor: where ecology and economics diverge. Ecol.
U
Econ. 48, 425-438.
AN
Azeredo, H. M.C.D., Pereira, A.C., Souza, A.C. R.D., Gouveia, S.T., Mendes, K.C.B., 2009.
Study on efficiency of betacyanin extraction from red beetroots. Int. J. Food Sci. Technol.
M
44, 2464-2469.
D
Baliarsingh, S., Panda, A.K., Jena, J., Das, T., Das, N.B., 2012. Exploring sustainable
EP
technique on natural dye extraction from native plants for textile: identification of
colorants, colorimetric analysis of dyed yarns and their antimicrobial evaluation. J. Clean.
C
Barani, H., Maleki, H., 2011. Plasma and Ultrasonic Process in Dyeing of Wool Fibers with
Bao-Qi, L., Xiao-Peng, Z., Wei, L., 2008. The synergistic effect of two photosynthetic
pigments in dye-sensitized mesoporous TiO2 solar cells. Dyes Pigments 76, 327-31.
39
ACCEPTED MANUSCRIPT
Bazargan, M.H., 2010. Performance of nano structured dye-sensitized solar cell utilizing
natural sensitizer operated with platinum and carbon coated counter electrodes. Int. J.
Bechtold, T., Mahmud-Ali, A., 2008. Efficient processing of raw material defines the
PT
ecological position of natural dyes in textile production. Int. J. Environ. Waste Manage. 2,
RI
215-232.
SC
Bechtold, T., MahmudAli, A., Mussak, R.A., 2007a. Reuse of ashtree (Fraxinus excelsior
U
AN
L.) bark as natural dyes for textile dyeing: process conditions and process stability. Color.
M
Technol. 123, 271-279.
D
TE
Bechtold, T., MahmudAli, A., Mussak, R., 2007b. Anthocyanin dyes extracted from grape
C EP
pomace for the purpose of textile dyeing. J. Sci. Food Agric. 87, 2589-2595.
AC
Bechtold, T., Mahmud-Ali, A., Komboonchoo, S., 2009. Sustainable dyes from Agri-Food
Chain co-products, in: Walden, K.W., Moates, Faulds, C.B. (Eds.), Total Food. RSC
40
ACCEPTED MANUSCRIPT
Bechtold, T., Mussak, R., MahmudAli, A., Ganglberger, E., Geissler, S., 2006. Extraction of
PT
natural dyes for textile dyeing from coloured plant wastes released from the food and
RI
beverage industry. J. Sci. Food Agric.86, 233-242.
SC
Bechtold, T., Turcanu, A., Ganglberger, E., Geissler, S., 2003. Natural dyes in modern textile
dyehouses how to combine experiences of two centuries to meet the demands of the
U
future? J. Clean. Prod. 11, 499509.
AN
Bechtold, T., Turcanu, A., Geissler, S., Ganglberger, E., 2002. Process balance and product
quality in the production of natural indigo from Polygonum tinctorium Ait. Applying low-
M
technology methods. Biores. Technol. 81, 171-177.
D
Beutner, S., Bloedorn, B., Frixel, S., Blanco, I.H., Hoffmann, T., Martin, H.D., Mayer, B.,
TE
Noack, P., Ruck, C., Schmidt, M., Schlke, I., Sell, S., Ernst, H., Haremza, S., Seybold,
G., Sies, H., Stahl, W., Walsh, R., 2001. Quantitative assessment of antioxidant properties
EP
The role of -carotene in antioxidant functions. J. Sci. Food Agric. 81, 559-568.
C
Bhattacharya, N., Lohiya, N., 2002. Dyeing of cotton and polyester fiber with pomegranate
AC
rind, catechu, nova red and turmeric. Asian Text. J. 11, 70-74.
Bhatti, I.A., Adeel, S., Jamal, A., Safdar, M., Abbas, M., 2010. Influence of gamma radiation
on the colour strength and fastness properties of fabric using turmeric (Curcuma longa L.)
41
ACCEPTED MANUSCRIPT
Bhuyan, R., Saikia, C.N., 2005. Isolation of colour components from native dye-bearing
Boo, H.O., Hwang, S.J., Bae, C.S., Park, S.H., Heo, B.G., Gorinstein, S., 2012. Extraction
and characterization of some natural plant pigments. Ind. Crop. Prod. 40, 129-135
PT
Boonsong, P., Laohakunjit, N., Kerdchoechuen, O., 2012. Natural pigments from six species
RI
of Thai plants extracted by water for hair dyeing product application. J. Clean. Prod. 37,
93-106.
SC
Borges, M.E., Tejera, R.L., Diaz, L., Esparza, P., Ibanez, E., 2012. Natural dyes extraction
U
from cochineal (Dactylopius coccus). New extraction methods. Food Chem. 132, 1855
1860. AN
Bruni, S., Guglielmi, V., Pozzi, F., Mercuri, A.M., 2011. Surface-enhanced Raman
M
spectroscopy (SERS) on silver colloids for the identification of ancient textile dyes. Part
Burrows, J.D., 2009. Palette of our palates: A brief history of food coloring and its regulation.
Bulut, M.O., Akar, E., 2012. Ecological dyeing with some plant pulps on woolen yarn and
Burkinshaw, S.M., Kumar, N., 2009. The mordant dyeing of wool using tannic acid and
AC
Calis, A., Celik, G.Y., Katircioglu, H., 2009. Antimicrobial effect of natural dyes on some
42
ACCEPTED MANUSCRIPT
Calogero, G., Marco, G.D., 2008. Red Sicilian orange and purple eggplant fruits as natural
sensitizers for dye-sensitized solar cells. Sol. Energ. Mater. Sol. Cells 92, 1341 1346.
Calogero, G., Marco, G.D., Caramori, S., Cazzanti, S., Argazzi, R., Bignozzi, C.A., 2009.
Natural dye senstizers for photoelectrochemical cells. Energy Environ. Sci.2, 1162-1172.
PT
Calogero, G., Marco, G.D., Cazzanti, S., Caramori, S., Argazzi, R., Carlo, A.D., Bignozzi,
RI
C.A., 2010. Efficient Dye-Sensitized Solar Cells Using Red Turnip and Purple Wild
SC
Calogero, G., Yum, J.H., Sinopoli, A., Marco, G.D., Grtzel, M., Nazeeruddin, M.K., 2012.
U
Anthocyanins and betalains as light-harvesting pigments for dye-sensitized solar cells.
Highly Efficient Porphyrin Sensitizers for Dye-Sensitized Solar Cells. J. Phys. Chem. C
D
111, 11760-11762.
TE
Campo, J.A.D., Garcia Gonzalez, M., Guerrero, M.G., 2007. Outdoor cultivation of
EP
microalgae for carotenoid production: current state and perspectives. Appl. Microbiol.
Caniato, F., Caridi, M., Crippa, L., Moretto, A., 2012. Environmental sustainability in fashion
AC
supply chains: An exploratory case based research. Int. J. Prod. Econ. 135, 659-670.
Galn-Vidal, C.A., 2009. Chemical studies of anthocyanins: A review. Food Chem. 113,
859-871.
43
ACCEPTED MANUSCRIPT
Castellar, M.R., Obon, J.M., Alacid, M., Fernaandez-Loopez, J.A., 2008. Fermentation of
Opuntia stricta (Haw.) Fruits for Betalains Concentration. J. Agric. Food Chem. 56,
42534257.
Chairat, M., Bremner, J.B., Chantrapromma, K., 2007. Dyeing of Cotton and Silk Yarn with
PT
the Extracted Dye from the Fruit Hulls of Mangosteen, Garcinia mangostana Linn. Fiber.
RI
Polym. 8, 613-619.
Chairat, M., Darumas, U., Bremner, J.B., Bangrak, P., 2011. Dyeing of cotton yarn with the
SC
aqueous extract of the leaves of Eupatorium odoratum L. in Thailand and associated
U
AN
Chang, H., Lo, Y.J., 2010. Pomegranate leaves and mulberry fruit as natural sensitizers for
solar cell using natural dyes extracted from spinach and ipomoea. J. Alloy. Compd. 495,
D
606-610.
TE
Chattopadhyay, P., Chatterjee, S., Sen, S.K., 2008. Biotechnological potential of natural food
C
Chattopadhyay, S.N., Pan, N.C., Roy, A.K., Saxena, S., Khan, A., Development of natural
dyed jute fabric with improved colour yield and UV protection characteristics. J. Text. I.
(2013) http://dx.doi.org/10.1080/00405000.2012.758352
44
ACCEPTED MANUSCRIPT
Chen, C., Chang, W.Y., 2007. Antimicrobial activity of cotton fabric pretreated by
microwave plasma and dyed with onion skin and onion pulp extractions. Indian J. Fibre
Chigurupati, N., Saiki, L., Gayser Jr, C., Dash, A.K., 2002. Evaluation of red cabbage dye as
PT
a potential natural color for pharmaceutical use. Int. J. Pharm. 241, 293299.
RI
Cho, M.H., Paik, Y.S., Hahn, T.R., 2000. Enzymatic Conversion of Precarthamin to
Carthamin by a Purified Enzyme from the Yellow Petals of Safflower. J. Agric. Food
SC
Chem. 48, 3917-3921.
U
Cristea, D., Vilarem, G., 2006. Improving light fastness of natural dyes on cotton yarn. Dyes
Cushnie, T.P.T., Lamb, A.J., 2005. Antimicrobial activity of flavonoids. Int. J. Antimicrob.
Dai, Q., Rabani, J., 2001. Photosensitization of nanocrystalline TiO2 films by pomegranate
pigments with unusually high efficiency in aqueous medium. Chem. Commun. 2142-
C
2143.
AC
Dai, Q., Rabani, J., 2002. Unusually efficient photosensitization of nanocrystalline TiO2 films
Das, D., Maulik, S.R., Bhattacharya, S.C., 2008. Colouration of wool and silk with Rheum
45
ACCEPTED MANUSCRIPT
Dawson, T.L., 2008. It must be green: meeting societys environmental concerns. Color.
Dawson, T.L., 2009. Biosynthesis and synthesis of natural colours. Color. Technol. 125, 61
73.
PT
Delgado-Vargas, F., Jimenez, A.R., Paredes-Lopez, O., 2000. Natural Pigments: Carotenoids,
RI
Anthocyanins, and Betalains Characteristics, Biosynthesis, Processing, and Stability.
SC
Dev, V.R.G., Venugopal, J., Sudha, S., Deepika, G., Ramakrishna, S., 2009. Dyeing and
U
antimicrobial characteristics of chitosan treated wool fabrics with henna dye. Carbohydr.
Downham, A., Collins, P., 2000. Colouring our foods in the last and next millennium. Int. J.
TE
Dufosse, L., 2006. Microbial Production of Food Grade Pigments. Food Technol. Biotechnol.
EP
44, 313321.
C
Dufosse, L., Galaup, P., Yaron, A., Arad, S.M., Blanc, P., Murthy, K.N.C., Ravishankar,
G.A., 2005. Microorganisms and microalgae as sources of pigments for food use: a
AC
scientific oddity or an industrial reality? Trends Food Sci. Tech. 16, 389406.
Duran, N., Duran, M., 2000. Enzyme applications in the textile industry. Rev. Prog.
46
ACCEPTED MANUSCRIPT
Duran, N., Teixeira, M.F., Conti R.D., Esposito E., 2002. Ecological-friendly pigments from
Dweck, A.C., 2002. Natural ingredients for colouring and styling. Int. J. Cosmetic Sci. 24,
287-302.
PT
Dweck, A. C., 2009a. Nature provides huge range of colour possibilities. Personal Care. June,
RI
61-73.
SC
Dweck, A. C., 2009b. Comprehensive focus on natural dyes. Personal Care. September, 57-
69.
U
El-Shishtawy, R.M., Shokry, G.M., Ahmed, N.S.E., Kamel, M.M., 2009. Dyeing of
AN
Modified Acrylic Fibers with Curcumin and Madder Natural Dyes. Fiber. Polym. 10,
617-624.
M
Espinosa, R., Zumeta, I., Santana, J.L., Martinez-Luzardo, F., Gonzalez, B., Docteur, S.,
D
Vigil, E., 2005. Nanocrystalline TiO2 photosensitized with natural polymers withenh
TE
anced efficiency from 400 to 600nm. Sol. Energ. Mat. Sol. Cells 85, 359369.
Feng, X.X., Zhang, L.L., Chen J.Y., Zhang, J.C., 2007. New insights into solar UV-protective
EP
Frick, D., 2003. The coloration of food. Rev. Prog. Color. 33, 15-32.
Furukawa, S., Iino, H., Iwamoto, T., Kukita, K., Yamauchi, S., 2009. Characteristics of dye-
sensitized solar cells using natural dye. Thin Solid Films 518, 526-529.
47
ACCEPTED MANUSCRIPT
Gao, Y., Cranston, R., 2008. Recent advances in antimicrobial treatment of textiles. Text.
Garcia, C.G., Polo, A.S., Iha, N.Y.M., 2003a. Fruit extracts and ruthenium polypyridinic dyes
PT
Chem. 160, 87-91.
RI
Garcia, C.G., Polo, A.S., Iha, N.Y.M., 2003b. Photoeletrochemical solar cell using extract of
Eugenia jambolana Lam as a natural sensitizer. An. Acad. Bras. Cienc. 75, 163-165.
SC
Ghoranneviss, M., Shahidi, S., Anvari, A., Motaghi, Z., Wiener, J., Slamborova, I., 2011.
U
Influence of plasma sputtering treatment on natural dyeing and antibacterial activity of
AN
wool fabrics. Prog. Org. Coat. 70, 388393.
Ghouila, H., Meksi, N., Haddar, W., Mhennib, M.F., Jannet, H.B., 2012. Extraction,
M
identification and dyeing studies of Isosalipurposide, a natural chalcone dye from Acacia
264274.
EP
Ganglberger, E., 2009. Environmental Aspects and Sustainability. in: Bechtold, T., Mussak,
R. (Eds.), Handbook of Natural Colorants, John Wiley & Sons, Ltd., Chichester, UK, pp.
C
353-366.
AC
Geissler, S., 2009. Economic Aspects of Natural Dyes. in: Bechtold, T., Mussak, R. (Eds.),
Handbook of Natural Colorants, John Wiley & Sons, Ltd., Chichester, UK, pp. 367-384.
Gilbert, K.G., Cooke, D.T., 2001. Dyes from plants: Past usage, present understanding and
48
ACCEPTED MANUSCRIPT
Gowacki, E.D., Voss, G., Leonat, L., Irimia-Vladu, M., Bauer, S., Sariciftci, N.S., 2012.
Indigo and Tyrian Purple From Ancient Natural Dyes to Modern Organic
Goktas, O., Duru, M.E., Yeniocak, M., Ozen, E., 2008. Determination of the color stability of
PT
an environmentally friendly wood stain derived from laurel (Laurus nobilis L.) leaf
RI
extracts under UV exposure, Forest Prod. J. 58, 77-80.
SC
Azamar-Barrios, J.A., Oskam, G., 2010. Dye-sensitized solar cells with natural dyes
extracted from achiote seeds. Sol. Energ. Mat. Sol. Cells 94, 4044.
U
AN
Gonzalez, M., Mendez, J., Carnero, A., Lobo, M.G., Afonso, A., 2002. Optimizing
Grifoni, D., Bacci, L., Zipoli, G., Carreras, G., Baronti, S., Sabatini, F., 2009. Laboratory and
Outdoor Assessment of UV Protection Offered by Flax and Hemp Fabrics Dyed with
EP
Grifoni, D., Bacci, L., Zipoli, G., Albanese, L., Sabatini, F., 2011. The role of natural dyes in
C
the UV protection of fabrics made of vegetable fibres. Dyes Pigments 91, 279-285.
AC
Guesmi, A., Hamadi, N.B., Ladhari, N., Sakli, F., 201a. Isolation, identification and dyeing
studies of betanin on modified acrylic fabrics. Ind. Crop. Prod. , 37, 342-346
Guesmi, A., Hamadi, N.B., Ladhari, N., Sakli, F., 2012b. Dyeing properties and colour
fastness of wool dyed with indicaxanthin natural dye. Ind. Crop. Prod. 37, 493-499.
49
ACCEPTED MANUSCRIPT
Guesmi, A., Hamadi, N.B., Ladhari, N., Sakli, F., 2013. Sonicator dyeing of modified acrylic
fabrics with indicaxanthin natural dye. Ind. Crop. Prod. 42, 63-69.
Guinot, P., Roge, A., Gargadennec, A., Garcia, M., Dupont, D., Lecoeur, E., Candelier, L.,
Andary, C., 2006. Dyeing plants screening: an approach to combine past heritage and
PT
present development. Color. Technol. 122, 93101.
RI
Gupta, D., Khare, S.K., Laha, A., 2004. Antimicrobial properties of naturel dyes against
SC
Gupta, D., Jain, A., Panwar, S., 2005. Anti-UV and anti-microbial properties of some natural
U
dyes on cotton. Indian J. Fibre Text. Res.30, 190-195.
AN
Gupta, D., Laha, A., 2007. Antimicrobial activity of cotton fabric treated with Quercus
32, 254-263.
TE
Haji, A. 2010. Functional Dyeing of Wool with Natural Dye Extracted from Berberis vulgaris
Wood and Rumex Hymenosepolus Root as Biomordant. Iran. J. Chem. Chem. Eng.
EP
29(3), 55-60.
C
Han, S., Yang, Y., 2005. Antimicrobial activity of wool fabric treated with curcumin. Dyes
Hao, S., Wu, J., Huang, Y., Lin, J., 2006. Natural dyes as photosensitizers for dye-sensitized
50
ACCEPTED MANUSCRIPT
Hebeish, A.A., Ragheb, A.A., Nassar, S.H., Allam, E.E., Thalouth, J.I.A.E., 2006.
Heera, T.R., Cindrella, L., 2010. Molecular orbital evaluation of charge flow dynamics in
PT
natural pigments based photosensitizers. J. Mol. Model. 16, 523533.
RI
Hemalatha, K.V., Karthick, S.N., Raj, C.J., Hong, N.Y., Kim, S.K., Kim, H.J., 2012.
Performance of Kerria japonica and Rosa chinensis flower dyes as sensitizers for dye-
SC
sensitized solar cells. Spectrochim. Acta A 96, 305-309.
U
Henry, B.S., 2000. Health aspects of Natural Colors, in: Lauro, G.J., Francis, F.J. (Eds.),
AN
Natural Food Colorants. Mark Dekker Inc., New York., USA, pp. 315-327.
Herbach, K. M., Stintzing, F.C., Carle, R., 2006. Betalain Stability and Degradation
M
Structural and Chromatic Aspects. J. Food Sci. 71, R41-R50.
D
Hill, D.J., 1997. Is there future in natural dyes? Rev. Prog. Coloration 27, 18-25.
TE
Holme, I., 2006. Sir William Henry Perkin: a review of his life, work and legacy. Color.
Hong, K.H., Bae, J.H., Jin, S.R., Yang, J.S., 2012. Preparation and properties of multi
C
functionalized cotton fabrics treated by extracts of gromwell and gallnut. Cellulose 19,
507515.
AC
Hou, X., Chen, X., Cheng, Y., Xu, H., Chen, L., Yang, Y., Dyeing and UV-protection
http://dx.doi.org/10.1016/j.jclepro.2013.03.004
51
ACCEPTED MANUSCRIPT
Humphrey, A.M., 2004. Chlorophyll as a Color and Functional Ingredient. J. Food Sci. 69,
C422-C425.
Hustvedt, G., Crews, P.C., 2005. The Ultraviolet Protection Factor of Naturally-pigmented
PT
Hwang, E.K., Lee, Y.H., Kim, H.D., 2008. Dyeing, Fastness, and Deodorizing Properties of
RI
Cotton, Silk, and Wool Fabrics Dyed with Gardenia, Coffee Sludge, Cassia tora. L., and
SC
Ibrahim, N.A., El-Gamal, A.R., Gouda, M., Mahrous, F., 2010. A new approach for natural
U
dyeing and functional finishing of cotton cellulose. Carbohydr. Polym. 82, 1205-1211.
AN
Ikegami, M., Ozeki, M., Kijitori, Y., Miyasaka, T., 2008. Chlorin-sensitized high-efficiency
photovoltaic cells that mimic spectral response of photosynthesis. Electrochem. 76, 140-
M
143.
D
Iqbal, J., Bhatti, I.A., Adeel, S., 2008. Effect of UV radiation on dyeing of cotton fabric with
TE
Irimia-Vladu, M., Gowacki, E.D., Troshin, P.A., Schwabegger, G., Leonat, L., Susarova,
EP
D.K., Krystal, O., Ullah, M., Kanbur, Y., Bodea, M.A., Razumov, V.F., Sitter, H., Bauer,
S., Sariciftci, N.S., 2012. Indigo - A Natural Pigment for High Performance Ambipolar
C
Organic Field Effect Transistors and Circuits. Adv. Mat. 24, 375-380.
AC
Ismal, O.E., Yildirim, L., 2012. Almond shell as a natural colorant. Indian J. Fibre Text. Res.
37, 358-363.
52
ACCEPTED MANUSCRIPT
Ito, S., Saitou, T., Imahori, H., Uehara, H., Hasegawa, N., 2010. Fabrication of dye-sensitized
solar cells using natural dye for food pigment: Monascus yellow. Energy Environ. Sci. 3,
905-909.
Janhom, S., Griffiths, P., Watanesk, R., Watanesk, S., 2004. Enhancement of lac dye
PT
adsorption on cotton fibres by poly(ethyleneimine). Dyes Pigments 63, 231-237.
RI
Janhom, S., Watanesk, R., Watanesk, S., Griffiths, P., Arquero, O.A., Naksata, W., 2006.
Comparative study of lac dye adsorption on cotton fibre surface modified by synthetic
SC
and natural polymers. Dyes Pigments 71, 188-193.
U
Jo, R.A., Casal, M., Cavaco-Paulo, A., 2008. Application of enzymes for textile fibres
AN
processing. Biocatal. Biotransfor. 26, 332-349.
Joshi, M., Ali, S.W., Purwar, R., Rajendran, S., 2009. Ecofriendly antimicrobial finishing of
M
textiles using bioactive agents based on natural products. Indian J. Fibre Text. Res. 34,
295-304.
D
TE
Kadolph, S.J., 2008. Natural Dyes: A Traditional Craft Experiencing New Attention. Delta
Kadolph, S. J., Casselman, K.D., 2004. In the Bag: Contact Natural Dyes. Cloth. Text. Res. J.
22, 15-47.
C
Kamel, M.M., El-Shishtawy, R.M., Yussef, B.M., Mashaly, H., 2005. Ultrasonic assisted
AC
dyeing III. Dyeing of wool with lac as a natural dye. Dyes Pigments 65, 103-110.
Kamel, M.M., El-Shishtawy, R.M., Yussef, B.M., Mashaly, H., 2007. Ultrasonic assisted
dyeing. IV. Dyeing of cationised cotton with lac natural dye. Dyes Pigments 73, 279-284.
53
ACCEPTED MANUSCRIPT
Kamel, M.M., El-Zawahry, M.M., Ahmed, N.S.E., Abdelghaffar, F., 2009a. Ultrasonic
dyeing of cationized cotton fabric with natural dye. Part 1: Cationization of cotton using
Kamel, M.M., El-Zawahry, M.M., Ahmed, N.S.E., Abdelghaffar, F., 2011. Ultrasonic dyeing
PT
of cationized cotton fabric with natural dye. Part 2: Cationization of cotton using Quat
RI
188. Ind. Crop. Prod. 34, 1410-1417.
Kamel, M.M., Helmy, H.M., El-Hawary, N.S., 2009b. Some studies on dyeing properties of
SC
cotton fabrics with Crocus sativus (saffron) (flowers) using an ultrasonic method,
U
AN
Kapoor, V.P., 2005. Herbal cosmetics for skin and hair care. Nat. Prod. Rad. 4, 306-314.
Kapoor, V.P., Katiyar, K., Pushpangadan, P., Singh, N., 2008. Development of Natural dye
M
based Sindoor. Nat. Prod. Rad. 7, 22-29.
D
Kavitha, T., Padmashwini, R., Swarna, A., Dev, V.R.G., Neelakandan, R., 2007. Effect of
TE
chitosan treatment on the properties of turmeric dyed cotton yarn. Ind. J. Fibre Text. Res.
32, 53-56.
EP
Kato, H., Hata T., Tsukada, M., 2004. Potentialities of Natural Dyestuffs as Antifeedants
against Varied Carpet Beetle, Anthrenus verbasci. Jpn. Agr. Res. Q. 38, 241-251.
C
Ke, G., Yu, W., Yu, W., 2006. Color evaluation of wool fabric dyed with Rhizoma coptidis
AC
Kerkeni, A., Behary, N., Perwuelz, A., Gupta, D., 2012. Dyeing of woven polyester fabric
with curcumin: effect of dye concentrations and surface pre-activation using air
atmospheric plasma and ultraviolet excimer treatment. Color. Technol. 128, 223-229.
54
ACCEPTED MANUSCRIPT
Khan, M.I., Ahmad, A., Khan, S.A., Yusuf, M., Shahid, M., Manzoor, N. Mohammad, F.,
2011. Assessment of antimicrobial activity of Catechu and its dyed substrate. J. Clean.
Khan, S.A., Ahmad, A., Khan, M.I., Yusuf, M., Shahid, M., Manzoor, N. Mohammad, F.,
PT
2012. Antimicrobial activity of wool yarn dyed with Rheum emodi L. (Indian Rhubarb).
RI
Dyes Pigments 95, 206-214.
Khan, P.M.A., Farooqui, M., 2011. Analytical Applications of Plant Extract as Natural pH
SC
Indicator: A Review. J. Adv. Scient. Res. 2(4), 20-27.
U
Kim, S., 2006. Dyeing characteristics and UV protection property of green tea dyed cotton
AN
fabrics: Focusing on the effect of chitosan mordanting condition. Fiber. Polym. 7, 255
261.
M
Kim, H., Park, S., 2007. Effects of introduced chemical groups on the dyeability of cotton
Kim, T.K., Son, Y.A., 2005. Effect of reactive anionic agent on dyeing of cellulosic fibers
with a Berberine colorantd part 2: anionic agent treatment and antimicrobial activity of a
EP
Kim, T.K., Yoon, S.H., Son, Y.A., 2004. Effect of reactive anionic agent on dyeing of
C
Kohno, Y., Totsuka, K., Ikoma, S., Yoda, K., Shibata, M., Matsushima, R., Tomita, Y.,
Maeda, Y., Kobayashi, K., 2009. Photostability enhancement of anionic natural dye by
55
ACCEPTED MANUSCRIPT
Komboonchoo, S., Bechtold, T., 2009. Natural dyeing of wool and hair with indigo carmine
(C.I. Natural Blue 2), a renewable resource based blue dye. J. Clean. Prod. 17, 1487-
1493.
Kong, W., Liu, N., Zhang, J., Yang, Q., Hua, S., Song, H., Xia, C., Optimization of
PT
ultrasound-assisted extraction parameters of chlorophyll from Chlorella vulgaris residue
RI
after lipid separation using response surface methodology. J. Food Sci. Technol. (2012)
http://dx.doi.org/10.1007/s13197-012-0706-z
SC
Kumbasar, E.P.A., Atav, R., Bahtiyari, M.I., 2009. Effects of Alkali Proteases on Dyeing
Properties of Various Proteinous Materials with Natural Dyes. Text. Res. J. 79, 517-525.
U
AN
Kumar, J.K., Sinha, A.K., 2004. Resurgence of natural colourants: a holistic view. Nat. Prod.
2006. Shiso leaf pigments for dye -sensitized solid-state solar cell. Sol. Energ. Mat. Sol.
D
Kuswandi, B., Jayus, Larasati, T.S., Abdullah, A., Heng, L.Y., 2012. Real-Time Monitoring
EP
Lai, W.H.; Su, Y.H.; Teoh, L.G.; Hon, M.H., 2008. Commercial and natural dyes as
AC
Lee, Y.H., Hwang, E.K., Jung, Y.J., Do, S.K, Kim, H.D., 2008. Dyeing and Deodorizing
Properties of Cotton, Silk, Wool Fabrics Dyed with Amur Corktree, Dryopteris
56
ACCEPTED MANUSCRIPT
2246-2253.
Lee, Y.H., Hwang, E.K., Kim, H.D., 2009. Assay and Antibacterial Activity of Cotton, Silk,
and Wool Fabrics Dyed with Peony, Pomegranate, Clove, Coptis chinensis and Gallnut
PT
extracts. Materials 2, 10-21.
Lee, Y.H., Kim, H.D., 2004. Dyeing Properties and Colour Fastness of Cotton and Silk
RI
Fabrics Dyed with Cassia tora L. Extract. Fiber. Polym. 5, 303-308.
SC
Lee, J.J., Lee, H.H., Eom, S.I., Kim, J.P., 2001. UV absorber aftertreatment to improve
U
Lewis, N.S., Nocera, D.G., 2006. Powering the planet: Chemical challenges in solar energy
AN
utilization. P. Natl. Acad. Sci. USA, 103, 15729-15735.
Kyriakides, M.L., Tsatsaroni, E., Laderos, P., Georgiadou, K., 1998. Dyeing of cotton and
M
wool fibres with pigments from Crocus Sativus - effect of enzymatic treatment. Dyes
Lin, S.M., Lin, B.H., Hsieh, W.M., Ko, H.J., Liu, C.D., Chen, L.G., Chiou, R.Y., 2010.
TE
Longo, L., Vasapollo, G., 2005. Anthocyanins from bay (Laurus nobilis L.) berries. J. Agric.
Luo, P., Niu, H., Zheng, G., Bai, X., Zhang, M., Wang, W., 2009. From salmon pink to blue
AC
natural sensitizers for solar cells: Canna indica L., Salvia splendens, cowberry and
MacFoy, C., 2004. Ethonobotany and sustainable utilization of natural dye plants in Sierra
57
ACCEPTED MANUSCRIPT
Manhita, A., Ferreira, V., Vargas, H., Ribeiro, I., Candeias, A., Teixeira, D., Ferreira, T.,
Dias, C.B., 2011. Enlightening the influence of mordant, dyeing technique and
PT
Mansour, H.F., 2010. Environment and energy efficient dyeing of woollen fabric with Sticta
RI
Mansour, H. F., Heffernan, S., 2011. Environmental aspects on dyeing silk fabric with Sticta
SC
coronate lichen using ultrasonic energy and mild mordants. Clean Technol. Environ.
U
Mapari, S.A.S., Nielsen, K.F., Larsen, T.O., Frisvad, J.C., Meyer, A.S., Thrane, U., 2005.
AN
Exploring fungal biodiversity for the production of water-soluble pigments as potential
analysis of fungal pigments and natural food colorants. J. Agric. Food Chem. 54, 7028
D
7035.
TE
Mapari, S.A.S., Meyer, A.S., Thrane, U., Frisvad, J.C., 2009. Identification of potentially safe
promising fungal cell factories for the production of polyketide natural food colorants
EP
Mapari, S.A.S., Thrane, U., Meyer, A.S., 2010. Fungal polyketide azaphilone pigments as
C
Marcolino, V.A., Zanin, G.M., Durrant, L.R., Benassi, M.D.T., Matioli, G., 2011. Interaction
MGarrech, S., Ncib, F., 2009. Colorimetric study of effect of gamma-radiation on the color
of cotton fabric colored by henna dye. Appl. Radiat. Isot. 67, 20032006.
58
ACCEPTED MANUSCRIPT
Meksi, N., Haddar, W., Hammami, S., Mhenni, M.F., 2012. Olive mill wastewater: A
potential source of natural dyes for textile dyeing. Ind. Crop. Prod. 40, 103-109.
Meng, S., Ren, J., Kaxiras, E., 2008. Natural dyes adsorbed on TiO2 nanowire for
photovoltaic applications: enhanced light absorption and ultrafast electron injection. Nano
PT
Lett. 8, 32663272.
RI
Mikropoulou, E., Tsatsaroni, E., Varella, E.A., 2009. Revival of traditional European dyeing
SC
Mirjalili, M., Nazarpoor, K., Karimi, L., 2011. Eco-friendly dyeing of wool using natural dye
from weld as co-partner with synthetic dye. J. Clean. Prod. 19, 1045-1051.
U
Mishra, A., Daswal, S., 2007. Curcumin, a natural colorant as initiator for
AN
photopolymerization of styrene: kinetics and mechanism. Colloid. Polym. Sci. 285, 1109-
1117.
M
Mishra, P.K. Singh, P., Gupta, K.K., Tiwari, H., Srivastava, P., 2012. Extraction of natural
D
dye from Dahlia variabilis using ultrasound. Indian J. Fibre Text. Res. 37, 83-86.
TE
Moiz, A., Ahmed, M.A., Kausar, N., Ahmed, K., Sohail, M., 2010. Study the effect of metal
ion on wool fabric dyeing with tea as natural dye. J. Saudi Chem. Soc. 14, 69-76.
EP
Mongkholrattanasit, R., Krystufek, J., Wiener, J., 2010. Dyeing and Fastness Properties of
Natural Dyes Extracted from Eucalyptus Leaves Using Padding Techniques. Fiber.
C
Polym.11, 346-350.
AC
Mongkholrattanasit, R., Krystufek, J., Wiener, J., Vikova, M., 2011a. Dyeing, Fastness, and
UV Protection Properties of Silk and Wool Fabrics Dyed with Eucalyptus Leaf Extract by
59
ACCEPTED MANUSCRIPT
Mongkholrattanasit, R., Krystufek, J., Wiener, J., Vikova, M., 2011b. UV protection
properties of silk fabric dyed with eucalyptus leaf extract. J. Text. Inst. 102 (3), 272279.
Montazer, M., Parvinzadeh, M., 2004. Effect of Ammonia on Madder-Dyed Natural Protein
PT
Montazer, M., Parvinzadeh, M., Kiumarshi, A., 2004. Colorimetric properties of wool dyed
RI
with natural dyes after treatment with ammonia. Color. Technol. 120, 161-166.
SC
Montazer, M., Dadashian, F., Hemmatinejad, N., Farhoudi, K., 2009. Treatment of Wool
with Laccase and Dyeing with Madder. Appl. Biochem. Biotechnol. 158, 685693.
U
Mortensen, A., 2006. Carotenoids and other pigments as natural colorants. Pure Appl. Chem.
78, 14771491. AN
Mussak, R.A.M., Bechtold, T., 2009. Natural Colorants in Textile Dyeing, in: Bechtold, T.,
M
Mussak, R. (Eds.), Handbook of Natural Colorants, John Wiley & Sons, Ltd., Chichester,
Narayan, M.R., 2012. Review: Dye sensitized solar cells based on natural photosensitizers.
Narayanan, D.L., Saladi, R.N., Fox, J.L., 2010. Ultraviolet radiation and skin cancer. Int. J.
Nasirizadeh, N., Dehghanizadeh, H., Yazdanshenas, M.E., Moghadam, M.R., Karimi, A.,
AC
2012. Optimization of wool dyeing with rutin as natural dye by central composite design
Naz, S., Bhatti, I.A., Adeel, S., 2011. Dyeing properties of cotton fabric using un-irradiated
and gamma irradiated extracts of Eucalyptus camaldulensis bark powder. Indian J. Fibre
60
ACCEPTED MANUSCRIPT
Oda, H., 2012a. Improving light fastness of natural dye: photostabilisation of gardenia blue.
PT
Oda, H., 2012b. Improvement of light fastness of natural dye: effect of ultraviolet absorbers
RI
128, 108-113.
SC
Onal, A., Sari, A., Soylak, M., 2005. Ellagic acid from gallnut (Quercus infectoria):
Extraction and determination of its dyeing conditions for natural fibers. J. Sci. Ind. Res.,
U
64, 491-495.
AN
Oprea, C.I., Dumbrav, A., Enache, I., Georgescu, A., Gru, M.A., 2012. A combined
Park, J.H., Gatewood, B.M., Ramaswamy, G.N., 2005. Naturally Occurring Quinones and
TE
Flavonoid Dyes for Wool: Insect Feeding Deterrents. J. Appl. Polym. Sci. 98, 322328.
Park, K.H., Kim, T.Y., Park, J.Y., Jin, E.M., Yim, S.H., Fisher, J.G., Lee, J.W., 2013.
EP
Photochemical properties of dye-sensitized solar cell using mixed natural dyes extracted
Park, Y., Koo, K., Kim, S., Choe, J., 2008. Improving the Colorfastness of Poly(ethylene
AC
terephthalate) Fabrics with the Natural Dye of Caesalpinia sappan L. Wood Extract and
the Effect of Chitosan and Low-Temperature Plasma. J. Appl. Polym. Sc. 109, 160166.
Parvinzadeh, M., 2007. Effect of proteolytic enzyme on dyeing of wool with madder.
61
ACCEPTED MANUSCRIPT
Patrocinio, A.O.T., Mizoguchi, S.K., Paterno, L.G., Garcia, C.G., Iha, N.Y.M., 2009.
Efficient and low cost devices for solar energy conversion: Efficiency and stability of
Polo, A.S., Iha, N.Y.M., 2006. Blue sensitizers for solar cells: Natural dyes from Calafate and
PT
Jaboticaba. Sol. Energy Mater. Sol. Cells 90, 19361944.
RI
Prabhu, K.H., Teli, M.D., Eco-dyeing using Tamarindus indica L.seed coat tannin as a
natural mordant for textiles with antibacterial activity. J. Saudi Chem. Soc. (2011)
SC
http://dx.doi.org/10.1016/j.jscs.2011.10.014
U
Prabhu, K.H., Teli, M.D., Waghmare, N.G., 2011. Eco-Friendly Dyeing Using Natural
AN
Mordant Extracted from Emblica officinalis G. Fruit on Cotton and Silk Fabrics with
Study of Natural Dyes and Dyed Silk. J. Clean. Prod. 18, 1750-1756.
D
TE
Qin, C., Clark, A.E., 2007. DFT characterization of the optical and redox properties of natural
pigments relevant to dye-sensitized solar cells. Chem. Phys. Lett. 438, 2630.
EP
Raja, A.S.M., Thilagavathi, G., 2011. Influence of Enzyme and Mordant Treatments on the
Ramamoorthy, S., Mudgal, G., Rajesh, D., Khan, F.N., Vijayakumar, V., Rajasekaran, C.
AC
62
ACCEPTED MANUSCRIPT
Rao, Y.M., Shayeda, Sujatha, P., 2008. Formulation and evaluation of commonly used
Ratnapandian, S., Fergusson, S.M., Wang, L., 2012. Application of acacia natural dyes on
PT
Raturi, A., Fepuleai, Y., 2010. Photosynthesis in a test tube-dye sensitized solar cells as a
RI
teaching tool. Renew. Energ. 35, 1010-1013.
Reddy, A.L.M., Nagarajan, S., Chumyim, P., Gowda, S.R., Pradhan, P., Jadhav, S.R., Dubey,
SC
M., John, G., Ajayan, P.M., Lithium storage mechanisms in purpurin based organic
U
AN
Rekaby, M., Salem, A.A., Nassar, S.H., 2009. Eco-friendly printing of natural fabrics using
natural dyes from alkanet and rhubarb. J. Text. Institute 100, 486-495.
M
Robb, M.J., Ku, S.Y., Brunetti, F.G., Hawker, C.J., 2013. A renaissance of color: New
structures and building blocks for organic electronics. J. Polym. Sci A 51, 1263-1271.
D
TE
Roy, K., Gullapalli, S., Chaudhuri, U.R., Chakraborty, R., 2004. The use of a natural colorant
based on betalain in the manufacture of sweet products in India. Int. J. Food Sci. Technol.
EP
39, 1087-1091.
Sachan, K., Kapoor, V.P., 2007. Optimization of extraction and dyeing conditions for
C
Samanta, A.K., Agarwal, P., 2009. Application of natural dyes on textiles. Indian J. Fibre
63
ACCEPTED MANUSCRIPT
Samanta, A.K., Konar, A., Chakraborti, S., Datta, S., 2011. Dyeing of jute fabric with tesu
extract: Part 1 Effects of different mordants and dyeing process variables. Indian J.
Sandquist, C., McHale, J.L., 2011. Improved efficiency of betanin-based dye-sensitized solar
PT
cells. J. Photochem. Photobiol. A: Chem. 221, 9097.
RI
Sang-aroon, W., Saekow, S., Amornkitbamrung, V., 2012. Density functional theory study on
the electronic structure of Monascus dyes as photosensitizer for dye-sensitized solar cells.
SC
J. Photochemi. Photobiol. A: Chem. 236, 35 40.
U
Saranya, R., Jayapriya, J., Tamilselvi, A., 2012. Dyeing of silk fabric with phenazine from
AN
Pseudomonas species. Color. Technol. 128, 440-445.
Sarkar, A.K., 2004. An evaluation of UV protection imparted by cotton fabrics dyed with
M
natural colorant. BMC Dermatol. 4, 15.
D
Sarkar, A.K., 2007. On the relationship between fabric processing and ultraviolet radiation
TE
Sathiyanarayanan, M.P., Bhat, N.V., Kokate, S.S., Walnuj, V.E., 2010. Antibacterial finish
EP
for cotton fabric from herbal products. Indian J. Fibre Text. Res. 35, 50-58.
C
Savvidou M.I., Economides, D.G., 2007. Colour gamut produced by applying mixtures of
Savvidis, G., Zarkogianni, M., Karanikas, E., Lazaridis, N., Nikolaidis, N., Tsatsaroni, E.,
2013. Digital and conventional printing and dyeing with the natural dye annatto:
optimisation and standardisation processes to meet future demands. Color. Technol. 129,
55-63.
64
ACCEPTED MANUSCRIPT
Selvi, A.T., Aravindhan, R., Madhan, B., Rao, J.R., 2013. Studies on the application of
natural dye extract from Bixa orellana seeds for dyeing and finishing of leather. J. Clean
Senthil, T.S., Muthukumarasamy, N., Velauthapillai, D., Agilan, S., Thambidurai, M.,
PT
Balasundaraprabhu, R., 2011. Natural dye (cyanidin 3-O-glucoside) sensitized
RI
nanocrystalline TiO2 solar cell fabricated using liquid electrolyte/quasi-solid-state
SC
Shahid, M., Ahmad, A., Yusuf, M., Khan, M.I., Khan, S.A., Manzoor, N. Mohammad, F.,
2012. Dyeing, fastness and antimicrobial properties of woolen yarns dyed with gallnut
U
(Quercus infectoria Oliv.) extract. Dyes Pigments 95, 53-61.
AN
Shahidi, S., Ghoranneviss, M., 2011. Investigation on dye ability and antibacterial activity of
nanolayer platinum coated polyester fabric using DC magnetron sputtering. Prog. Org.
M
Coat. 70, 300303.
Shams-Nateri, A., 2011. Reusing wastewater of madder natural dye for wool dyeing. J.
D
solar cells fabricated with extracts from fruits of ivy gourd and flowers of red frangipani
EP
Sharma, D., Gupta, C., Aggarwal, S., Nagpal, N., 2012a. Pigment extraction form fungus for
C
Sharma, N., Kumar, R., Sinha, A.K., Reddy, P.B., Nayeem, S.M., Deep, S., 2012b.
Anthraquinone derivatives based natural dye from Rheum emodi as a probe for thermal
62, 96-104.
65
ACCEPTED MANUSCRIPT
Shekhawat, M.S., 2012. Studies on the Use of In vitro Synthesized Red Dye of Arnebia
PT
Shin, Y., Son, K., Yoo, D.I., 2010. Development of natural dyed textiles with thermo-
RI
Simoncic, B., Tomsic, B., 2010. Structures of novel antimicrobial agents for textiles-a
SC
review. Text. Res. J.80, 1721-1737.
Sinha, K., Saha, P.D., Datta, S., 2012. Response surface optimization and artificial neural
U
network modeling of microwave assisted natural dye extraction from pomegranate rind.
Singh, R., Jain, A., Panwar, S., Gupta, D., Khare, S.K., 2005. Antimicrobial activity of some
D
V., Tennakone, K., 2006. Utilization of natural pigment extracted from pomegranate
Siva, R., 2007. Status of natural dyes and dye yielding plants in India-An overview. Curr. Sci.
AC
92, 916-926.
Siva, R., Mathew, G.J., Venkat, A., Dhawan, C., 2008. An alternative tracking dye for gel
66
ACCEPTED MANUSCRIPT
Siva, R., Palackan, M.G., Maimoon, L., Geetha, T., Bhakta, D., Balamurugan, P.,
Sivakumar, V., Anna, J.L., Vijayeeswarri, J., Swaminathan, G., 2009. Ultrasound assisted
PT
enhancement in natural dye extraction from beetroot for industrial applications and
RI
natural dyeing of leather. Ultrason. Sonochem. 16, 782789.
Sivakumar, V., Vijaeeswarri, J., Anna, J.L., 2011. Effective natural dye extraction from
SC
different plant materials using ultrasound. Ind. Crop. Prod. 33, 116-122.
Smestad, G.P., 1998. Education and solar conversion: Demonstrating electron transfer. Sol.
U
Energ. Mat. .Sol. Cells 55, 157-178.
AN
Smestad, G.P., Gratzel, M., 1998. Demonstrating Electron Transfer and Nanotechnology: A
M
Natural DyeSensitized Nanocrystalline Energy Converter. J. Chem. Edu. 75, 752-756.
Son, Y.A., Kim, B.S., Ravikumar, K., Kim, T.K., 2007. Berberine Finishing for Developing
D
Sricharussin, W., Ree-iam, P., Phanomchoeng, W., Poolperm, S., 2009. Effect of enzymatic
EP
treatment on the dyeing of pineapple leaf fibres with natural dyes. ScienceAsia 35, 3136.
Stintzing, F.C., Carle, R., 2007. Betalains emerging prospects for food scientists. Trends
C
Tang, R.C., Tang, H., Yang, C., 2010. Adsorption Isotherms and Mordant Dyeing Properties
of Tea Polyphenols on Wool, Silk, and Nylon. Ind. Eng. Chem. Res. 49, 88948901
Thambidurai, M., Muthukumarasamy, N., Velauthapillai, D., Arul, N.S., Agilan, S.,
67
ACCEPTED MANUSCRIPT
solar cells with natural dyes extracted from Ixora coccinea, Mulberry and Beetroot. J
Thiry, M.C. 2011. Staying alive: Making Textiles Sustainable. AATCC Review Nov/Dec,
26-32.
PT
Tobin, L.L., OReilly, T., Zerulla, D., Sheridan, J.T., 2011. Characterising dye-sensitised
RI
Tousson, E., Al-Behbehani, B., 2011. Black mulberries (Morus nigra) as a natural dye for
SC
animal tissues staining, Anim. Biol. 61, 49-58.
Tsatsaroni, E., Kyriakides, M.L., Eleftheriadis, I., 1998. Comparative study of dyeing
U
properties of two yellow natural pigmentsEffect of enzymes and proteins. Dyes
Vankar, P.S., Sarswat, R., Dwivedi, A.K., An assessment and characterization for biosorption
TE
http://dx.doi.org/10.1016/j.jclepro.2011.09.021
EP
Vankar, P.S., Shanker, R., 2006. Sonicator dyeing of cotton and silk fabric by Ixora
C
Vankar, P.S., Shanker, R., 2008. Ecofriendly ultrasonic natural dyeing of cotton fabric with
Vankar, P.S., Shanker, R., 2009. Eco-friendly pretreatment of silk fabric for dyeing with
Vankar, P.S., Shanker, R., Dixit, S., Mahanta, D., Tiwari, S.C., 2008a. Sonicator Dyeing of
Natural Polymers with Symplocos spicata by Metal Chelation. Fiber. Polym. 9, 121-127.
68
ACCEPTED MANUSCRIPT
Vankar, P.S., Shanker, R., Dixit, S., Mahanta, D., Tiwari, S.C., 2008b. Sonicator dyeing of
cotton with the leaves extract Acer pectinatum Wallich. Pigm. Resin Technol. 37, 308
313.
Vankar, P.S., Shanker, R., Dixit, S., Mahanta, D., Tiwari, S.C., 2008c. Sonicator dyeing of
PT
modified cotton, wool and silk with Mahonia napaulensis DC. And identification of the
RI
Vankar, P.S., Shanker, R., Dixit, S., Mahanta, D., Tiwari, S.C., 2009a. Chemical
SC
characterisation of extract derived from Daphne papyraceae and sonicator dyeing of
cotton, silk and wool with the extract. Pigm. Resin Technol. 38, 181187.
U
Vankar, P.S., Shanker, R., Mahanta, D., Tiwari, S.C., 2008d. Ecofriendly sonicator dyeing of
AN
cotton with Rubia cordifolia Linn. using biomordants. Dyes Pigments 76, 207212.
Vankar, P.S., Shanker, R., Srivastava, J., 2007a. Ultrasonic dyeing of cotton fabric with
M
aqueous extract of Eclipta alba. Dyes Pigments 72, 33-37.
Vankar, P. S., Shanker, R., Verma, A. 2007b. Enzymatic natural dyeing of cotton and silk
D
Vankar, P.S., Tiwari, V., Singh L.W., Potsangbam, L., 2009b. Sonicator dyeing of cotton
Vankar, P.S., Tiwari, V., Srivastava, J., 2006. Extracts of stem bark of Eucalyptus globulus as
C
food dye with high antioxidant properties. Electron. J. Environ. Agric. Food Chem. 5,
AC
1664-1669.
Velmurugan, P., Chae, J.C., Lakshmanaperumalsamy, P., Yun, B.S., Lee, K.J., Oh, B.T.,
2009. Assessment of the dyeing properties of pigments from five fungi and anti-bacterial
activity of dyed cotton fabric and leather. Color. Technol. 125, 334341.
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Velmurugan, P., Lee Y.H., Nanthakumar, K., Kamala-Kannan, S., Dufosse, L., Mapari,
S.A., Oh, B.T., 2010. Water-soluble red pigments from Isaria farinosa and structural
Wakida, T., Cho, S., Choi, S., Tokino, S., Lee, M., 1998. Effect of Low Temperature Plasma
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Treatment on Color of Wool and Nylon 6 Fabrics Dyed with Natural Dyes. Text. Res. J.
68, 848-853.
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Wang, L., Wang, N., Jia S., Zhou, Q., 2009. Research on Dyeing and Ultraviolet Protection
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of Silk Fabric Using Vegetable Dyes Extracted from Flos Sophorae. Text. Res. J. 79,
14021409.
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Wang, C., Xu, C., Tian, A., Fu, S., Wang, C., 2012. Extraction of natural dyes from Alpinia
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blepharocalyx K. Schum. for dyeing of silk fabric. Color. Technol. 128, 1-7.
Wongcharee, K., Meeyoo, V., Chavadej, S., 2007. Dye-sensitized solar cell using natural
M
dyes extracted from rosella and blue pea flowers. Sol. Energ. Mat. Sol. Cells 91, 566
571.
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Wrolstad, R.E., Durst, R.W., Lee, J., 2005. Tracking color and pigment changes in
EP
Xinsheng, X., Lu, W., Shunhua, J., Qicheng, Z., 2008. Extraction of coloring matter from
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Sargentodoxa cuneata by ultrasonic technique and its application on wool fabric. Int. J.
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Yamazaki E., Murayama, M., Nishikawa, N., Hashimoto, N., Shoyama, M., Kurita, O., 2007.
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Yi, E., Cho, J.Y., 2008. Color Analysis of Natural Colorant-Dyed Fabrics. Color Res. Appl.
33, 148-157.
Yusuf, M., Ahmad, A., Shahid, M., Khan, M.I., Khan, S.A., Manzoor, N., Mohammad, F.,
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dyed with the extract of the leaves of henna (Lawsonia inermis). J. Clean. Prod. 27, 42-
50.
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Yusuf, M., Shahid, M., Khan, M.I., Khan, S.A., Khan, M. A., Mohammad, F., Dyeing studies
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with henna and madder: A research on effect of tin (II) chloride mordant. J. Saudi Chem.
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Zarkogianni, M., Mikropoulou, E., Varella, E., Tsatsaroni, E., 2011. Colour and fastness of
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natural dyes: revival of traditional dyeing techniques. Color. Technol., 127, 1827.
Zhang, D., Lanier, S.M., Downing, J.A., Avent, J.L., Lum, J., McHale, J.L., 2008. Betalain
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pigments for dye-sensitized solar cells. J. Photochem. Photobiol. A 195, 72-80.
Zhang, H., Zhan, J., Su, K., Zhang, Y., 2006. A kind of potential food additive produced
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Zhang, R., Cai, Z., 2011. Study on the Natural Dyeing of Wool Modified with Enzyme.
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Zheng, G.H., Fu, H.B., Liu, G.P., 2011. Application of rare earth as mordant for the dyeing of
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ramie fabrics with natural dyes. Korean J. Chem. Eng. 28, 2148-2155.
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Zhou, H., Wu, L., Gao, Y., Ma, T., 2011. Dye-sensitized solar cells using 20 natural dyes as
Zhu, H., Zeng, H., Subramanian, V., Masarapu, C., Hunga, K.H., Wei, B., 2008.
Anthocyanin-sensitized solar cells using carbon nanotube films as counter electrodes. 19,
465204-465208.
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Zyoud, A., Zaatar, N., Saadeddin, I., Helal, M.H., Campet, G., Hakim, M., Park, D.H., Hilal,
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Ferrous sulfate FeSO4.7H2O 2008a; Zarkogianni et al., 2011
Stannous chloride SnCl2.2H2O
Copper sulfate CuSO4.5H2O
Potassium dichromate K2Cr2O7
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Newly discovered metallic mordants
Magnesium sulphate MgSO4.7H2O Das et al., 2008; Moiz et al., 2010; Rekaby et al., 2009
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Aluminium sulphate Al2(SO4)3.13H2O Das et al., 2008; Hwang et al., 2008; Yi and Cho, 2008
Zinc sulphate ZnSO4.7H2O Ghouila et al., 2012; Guesmi et al., 2012a,b; Onal et al., 2005
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Nickel sulphate NiSO4.6H2O Hwang et al., 2008; Lee et al., 2004
Cobalt sulphate
Stannous sulphate
CoSO4.6H2O
SnSO4
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Ferric chloride FeCl3 Mikropoulou et al., 2009; Rekaby et al., 2009; Zarkogianni et al., 2011
Copper chloride
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Entada spiralis Chairat et al., 2007
Eucalyptus Sachan and Kapoor, 2007
Memecylon scutellatum Chairat et al., 2011
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Punica granatum Chattopadhyay et al., 2013
Quercus infectoria Grifoni et al., 2011
Rhus coriaria Bruni et al., 2011
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Rumex Hymenosepolus Haji, 2010
Tamarindus indica Prabhu and Teli, 2011
Terminalia bellerica Shekhawat, 2012
Terminalia chebula Samanta et al., 2011
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Prosopis spp. Shekhawat, 2012
Enterolobium cyclocarpum Arroyo-Figueroa et al., 2011
Caesalpinia coriaria
Symplococcus sp.
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Arroyo-Figueroa et al., 2011
Pyrus pashia Cu rich plant used as substitute Vankar and Shanker, 2009
of copper mordant
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Reference Enzyme Substrate Treatment Conditions Natural Dyes used in the study
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Class Trade Name Source pH Temp. Treatment Time
(oC) (Min)
Raja and Protease - - Wool 9 70 60 Grevillea robusta, Spathodea
Thilagavathi, campnulata, Cassia auriculata, Acacia
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2011 decurrens
Zhang and Cai, Protease Savinase 16L - Wool 8 50 45 Caesalpinia sappan
2011
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Transglutaminase - - 7 50 40
Montazer et al., Laccase Denilite II S - Wool 4.5 60 60 Rubia tinctorum
2009
Parvinzadeh, Protease Novolan T Bacillus sp. Wool 7 30 60 Rubia tinctorum
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Kumbasar et al., Protease Savinase Bacillus licheniformis Wool and 9-9.5 50 20 Rhus coriaria, Terminalia chebula, Quercus
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2009 Silk alba, Quercus infactoria
Alcalase Bacillus amyloliquefaciens 8-8.5 60 20
Vankar et al., Protease - Aspergillus oryzae Cotton 7.2 25 10 Terminalia Arjuna, Punica granatum,
2006; Vankar and silk Rheum emodi, Acacia catechu, Tectona
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Amylase - Aspergillus niger 7.1 30 10
and Shanker, 7.0 30 10
grandis, Delonix regia
Lipase - Aspergillus niger
2008, 2009
Diasterase - - 7.2 25 10
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Kyriakides et Amylase - - Cotton 7 - 10 Crocus sativus, Curcuma longa
al., 1998; Trypsin - - TE and Wool 8 - 30
Tsatsaroni et
al., 1998
- Not specified
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Electrode (mA/cm ) (V)
Red beet roots Betanin TiO2 caoted FTO Pt caoted FTO LiI/ I2/TBP 3-methoxyprpionitrile 2.42 0.44 0.63 0.67 Zhang et al., 2008
Betaxanthin Acetonitrile 2.00 0.22 0.51 0.19
Red cabbage:curcumin - TiO2 caoted FTO Pt coated ITO LiI/I2/DMPImI/TBP Propylene carbonate 0.81 0.53 0.69 0.60 Furukawa et al., 2009
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Red perilla Shisonin 0.39 0.51 0.67 0.27
Red cabbage - 0.56 1.55 0.67 1.17
Chaste tree fruit - TiO2 caoted FTO Pt caoted ITO LiI/I2 Acetonitrile/ 1.06 0.39 0.48 - Garcia et al., 2003
Morus alba - 3-methyl-2-oxazolidinone 0.86 0.422 0.43 -
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Euterpe oleraceaa - 0.37 0.442 0.61 -
Beta vulgaris rubra - TiO2 caoted FTO Pt caoted FTO LiI/ I2 3-methoxypropionitrile 9.5 0.425 0.35 1.7 Calogero et al., 2010
Opuntia engelmannii - 9.4 0.350 0.38 1.26
Opuntia ficus indica - 2.7 0.375 0.54 0.50
Bougainvillea - 2.1 0.300 0.57 0.36
Morus alba Anthocyanidins TiO2 caoted FTO Pt caoted FTO LiI/I2/pyridine Acetonitrile/propionitrile 6.1 0.49 0.52 - Patrocinio et al., 2009
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Vaccinium myrtillus Anthocyanidins 1.0 0.59 0.61 -
Mirtus caulifora Anthocyanidins 3.9 0.45 0.56 -
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Hibiscus surattensis Anthocyanin TiO2 caoted FTO Pt caoted FTO TBAI/I2 Acetonitrile/ethylene 5.45 0.392 0.535 1.14 Fernando and Senadeera,
Sesbania grandiflora - carbonate 4.40 0.406 0.569 1.02 2008
Hibiscus rosasinensis - 4.04 0.400 0.633 1.02
Nerium oleander - 2.46 0.408 0.591 0.59
Ixora macrothyrsa - 1.31 0.403 0.568 0.30
Rhododendron arboretum - 1.15 0.402 0.637 0.29
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Beet root Betailain TiO2 caoted FTO Pt caoted FTO KI/I2 Ethylene glycol/acetonitrile 2.95 0.357 0.3 0.402 Oprea et al., 2012
Citrus Sinensis Cyanine TiO2 caoted FTO Pt caoted FTO KI/I2 Ethylene glycol/acetonitrile 3.84 0.340 - 0.50 Calogero and Marco, 2008
Solanum melongena, L. Nasunin 3.4 0.350 - 0.40
Begonia - TiO2 caoted FTO Pt caoted FTO DMPImI/LiI/I2/ GT/TBP Acetonitrile 0.63 0.537 0.722 0.24 Zhou et al., 2011
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Tangerine peel - 0.74 0.592 0.631 0.28
Rhododendron - 1.61 0.585 0.609 0.57
Fructus lycii - 0.53 0.689 0.466 0.17
Marigold
Perilla
Herba artmisiae scopariae
-
-
-
TE 0.51
1.36
1.03
0.542
0.522
0.484
0.831
0.696
0.682
0.23
0.50
0.34
China Ioropetal - 0.84 0.518 0.626 0.27
Yellow rose - 0.74 0.609 0.571 0.26
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Flower knotweed - 0.60 0.554 0.627 0.21
Bauhinia tree - 0.96 0.572 0.66 0.36
Petunia - 0.85 0.616 0.605 0.32
Lithospermum - 0.14 0.337 0.585 0.03
Violet - 1.02 0.498 0.645 0.33
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Norbixin 0.38 0.53 0.64 0.13
Bixin ZnO caoted FTO 0.087 0.32 0.37 0.01
Norbixin 0.15 0.34 0.34 0.017
Black rice Anthocyanin TiO2 coated Pt coated KI/I2 Ethylene glycol/ 1.142 0.551 0.52 - Hao et al., 2006
Erythrina Carotenoid conductive glass conductive glass acetonitrile 0.776 0.484 0.55 -
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Rosa xanthina Anthocyanin 0.637 0.492 0.52 -
Kelp Chlorophyll 0.433 0.441 0.62 -
Capsicum Carotenoid 0.225 0.412 0.63 -
Myrtus cauliflora Anthcyanin TiO2 caoted FTO Pt caoted FTO LiI/I2 Acetonitrile/3-methyl-2- 9.0 0.59 0.54 - Polo and Iha, 2006
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Berberies buxifolia Anthocyanin oxazolidinone 6.2 0.47 0.36 -
Monascus purpereus Xanthomonascin_A TiO 2 caoted FTO Pt caoted FTO LiI/ BMII /I2/TBP Acetonitrile/valeronitrile 6.1 0.57 0.66 2.3 Ito et al., 2010
Gardinia fruit Crocin TiO2 caoted FTO Pt coated ITO KI/ I2 Ethylene carbonate/ 2.84 0.43 0.46 0.56 Yamazaki et al., 2007
Crocetin acetonitrile 0.45 0.58 0.60 0.16
Spinach extract Chlorophyll TiO2 caoted ITO Pt coated ITO - - 0.467 0.55 0.51 0.131 Chang et al., 2010
Ipomea leaf extract Chlorophyll 0.914 0.54 0.563 0.278
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Pomegranate leaf extract Chlorophyll - - - - 2.05 0.56 0.52 0.597 Chang and Lo, 2010
mulberry extract Anthocyanin 1.89 0.555 0.53 0.548
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Chlorophyll + anthocyanin 2.8 0.53 0.49 0.722
Ixora coccinea - ZnO caoted ITO Pt coated ITO LiI/I2 Acetonitrile 2.65 0.21 0.29 0.33 Thambidurai et al., 2011
Mulberry - 2.90 0.23 0.30 0.41
Beetroot - 2.30 0.2 0.3 0.28
Delonix regia cyanidin 3-O-glucoside TiO2 caoted ITO Pt coated ITO LiI/I2 Acetonitrile 1.33 0.30 0.39 0.317 Senthil et al., 2011
TiO2LiI/ I2/PEO/TBP 0.84 0.30 0.48 0.245
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Eugenia Jambolana Anthocyanidin LiI/I2 Acetonitrile 1.49 0.35 0.48 0.505
TiO2LiI/ I2/PEO/TBP 1.58 0.30 0.46 0.444
Bogainvillea brasiliensis - Au Nanoparticle Ag coated ITO Ce(NO3)3/Ce(NO3)3 Ethanol/water 5 0.249 0.364 0.454 Lai et al., 2008
loaded on
Garcinia suubelliptica - 6.48 0.322 0.331 0.691
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TiO2 caoted FTO
Ficus Reusa Linn. - 7.85 0.520 0.289 1.18
Rhoeo spathacea - 10.9 0.496 0.273 1.49
Black berry Anthocyanin TiO2 caoted FTO Nanocarbon TE KI/I2 Anhydrous ethylene glycol 10.6 0.33 0.42 1.46 Zhu et al., 2008
coated FTO
Beet root Betanin TiO2 caoted FTO Pt caoted FTO LiI/I2 Acetonitrile 13.91 0.36 0.56 2.71 Sandquist and McHale,
3-methoxyproprionitrile 8.61 0.44 0.61 2.22 2011
Hibiscus flowers Anthocyanins TiO2 coated FTO Graphite coated - - 0.289 0.403 0.525 - Tobin et al., 2011
FTO
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Gardenia Yellow extract Geniposide, Crocin, Crocetin TiO2 coated FTO Pt coated FTO DMPImP/LiI/I2/TBP 3-methoxypropionitrile 0.96 0.54 0.62 0.32 Park et al., 2013
Gardenia Blue extract Crocin and Crocetin 0.53 0.44 0.69 0.16
Kerria japonica Xanthophyll TiO2 coated FTO Pt coated FTO Iodolyte AN 50 (Solaronix) - 0.5597 0.5839 0.6775 0.22 Hemalatha et al., 2012
Rosa chinensis Anthocyanin 0.8017 0.5433 0.664 0.29
Ivy gourd fruits -carotene TiO2 coated FTO Pt coated FTO LiI/I2/TBP 2-methoxypropionitrile 0.24 0.644 0.49 0.076 Shanmugam et al., 2013
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Table 5: Approved naturally derived food Colorants in European Union (EU), Food and Drug Administration
(FDA) of USA and 7th Edition of Japans Specifications and Standards for Food Additives (JSSFA)
EU Name E-number USA Name U.S. CFR JSSFA Name Colours obtained
number
Curcumin E 100 Turmeric 73.600 Turmeric oleoresin and Yellow
Turmeric oleoresin 73.615 curcumin
Riboflavin E101 Riboflavin 73.450 - Yellow
Riboflavin-5-phosphate
Cochineal, carminic acid, E120 Cochineal extract, carmine 73.100 Cochineal extract and Pink to Red
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carmines carminic acid
Chlorophylls and E140 - Chlorophyll Green to olive
Chlorophyllins
Copper complexes of E141 Sodium Copper 73.125 - Bluish green
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Chlorophylls and chlorophyllin
Chlorophyllins
Caramels E150 (a-d) Caramel 73.85 Caramel (a-d) Brown
Vegetable carbon E153 - - Grey to black
Carotenes E160a Carrot oil 73.300 Carotene from carrot Golden yellow to
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-carotene 73.95 orange
Carotene from palm oil
Carotene from Dunaliella
Annatto, bixin, norbixin E160b Annatto extract 73.30 - Orange
Paprika extract, capsanthin, E160c Paprika, 73.340 Paprika color and Reddish orange
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capsorubin Paprika oleoresin 73.345 oleoresin
Lycopene E160d Tomato lycopene extract, 73.585 - Orange red
tomato lycopene
-apo-8-carotenal (C30)
Ethyl ester of b-apo-8-
E160e
E160f
concentrate
-apo-8-carotenal
-
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Reddish orange
Yellow/Orange
carotenic acid (C30)
Lutein E161b - Marigold color Golden Yellow
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Canthaxanthin E161g Canthaxanthin 73.75 - Orange pink
Beetroot red, betanin E162 Dehydrated beets (beet 73.40 Red beetroot Pink to red
powder)
Anthocyanins E163 Grape color extract 73.169 Grape skin color and Depending on pH gives
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Fig. 2. A schematic representation of enhanced resourse utilization and waste minimization in a natural textile dyeing
ENERGY
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W ATER CULTIVATION FORESTRY FOOD INDUSTRY
FERTILIZER
PESTICIDES
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e.g. Indigo, Madder,
W eld, Sawwort W ASTE = LEAVES
e.g. Teak, Eucalyptus
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W ASTE
e.g. Pressed berries, Pomegranate peel,
Onion peel, walnut husk,
CROP TIMBER INDUSTRY Olive mill waste water
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W ASTE = BARK
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can be e.g. Ash tree bark, Alder,
utilized as
Animal feed
Soil conditioner
W OOD FOOD &
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Adsorbent
BEVERAGES
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AND EXTRACTION AND STANDERDIZATION
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can be utilized as W aste Compost
DYESTUFF W aste Biofuel
Adsorbent
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ENERGY
W ATER DYEING PROCESS W ASTE W ATER
DYEING AUXILARIES
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Fig. 3. Chemical structures of the main constituents of the natural dyes used in functional finishing of
textiles
HO OH R1 R2
O
R1 =OCH3, R2 = OCH3 Curcumin
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R1=H, R2=CH3 Chrysophanol; R1=H, R2=CH2OH Aloe-emodin
R1 =OCH3, R2 =H Demethoxycurcumin R1=H, R2=COOH Rhein; R1=CH3, R2=OH Emodin;
R1 =R2 =H Bisdemethoxycurcumin R1=CH3, R2=OCH3 Physcion
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Weld (Reseda luteola) Eucalyptus (Eucalyptus globulus) Cutch (Acacia catechu)
R OH OH
OH OH
HO O
OH
HO O
HO O
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OH
OH
OH O
R Catechin
OH O
R= OH Luteolin R= OH Quercetin
R= H Apigenin R= OC12H22O9 Rutin
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Onion (Alium cepa) Flos sophorae (Sophora japonica) Gallnut (Quercus infectoria) &
HO O
OH
OH
HO
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O
OH
OH
Pomegranate (Punica granatum)
COOH
O
O OH
HO OH
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OH OC H O HO OH
OH O 12 22 9 HO O
OH O
Quercetin Rutin OH O
Gallic acid Ellagic acid
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N
O
CH 3
N OCH 3
H O
Indigo CH 3
OCH 3
O OH
OH
Berberine
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Shikonin
HO OH R3
HO O
O
HO COOH
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OH O CH 3 R2 O OH
OH
HO OH OH O R1=H, R2=H, R3=COOH Tectoquinone
OH Morol R1=OH, R2=OH, R3=CH3 Tectoleafquinone
Carminic acid
R3
O R4
R1=OH, R2=OH, R3=H, R4=H Alizarin; R1=OH, R2=OH, R3=H, R4=OH Purpurin O
R1=OH, R2=COOH, R3=OH, R4=OH Pseudopurpurin; R1=OH, R2=CH3, R3=OH, R4=H Rubiadin Lawsone
R1=H, R2=OH, R3=COOH, R4=OH Manjistin R1=H, R2=OH, R3=H, R4=OH Xanthopurpurin
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Many different kinds of applications of natural dyes are under active study.
Special attention has been given to recent developments in natural food colorants.
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Some newly discovered applications of natural dyes have also been highlighted.
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