Aplicações Corantes Naturais - Review

Journal of Cleaner Production 53 (2013) 310e331
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Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro
Review
Recent advancements in natural dye applications: a review

Mohammad Shahid, Shahid-ul-Islam, Faqeer Mohammad*
Department of Chemistry, Jamia Millia Islamia (A Central University), Jamia Nagar, New Delhi 110025, India
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 23 June 2012
Received in revised form
15 March 2013
Accepted 17 March 2013
Available online 3 April 2013
A vast array of colorants obtained from natural sources such as plants, insects/animals 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-effective technologies for their processing and
application have greatly aided in widening the scope of natural dyes in various traditional and advanced
application disciplines. This review encompasses a summary of research performed in last 15 years (1998
e2013) in different arenas of applications of natural dyes, with specic reference to technological
development in natural textile dyeing and use of natural dyes in functional nishing of textiles, food
coloration and dye-sensitized solar cells. In addition, some newly discovered applications of natural dyes
have also been discussed.
! 2013 Elsevier Ltd. All rights reserved.
Keywords:
Natural dyes
Mordants
Protective textiles
Dye-sensitized solar cells
Food coloration
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 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 ingredients (Dweck, 2002) and cosmetics (Frick, 2003). With
the discovery of synthetic 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). However, the application of a number of synthetic dyes
has detrimental effects on environment and associated allergic,
toxic, carcinogenic, harmful responses. Amidst growing environmental and health concerns eco-friendly non-toxic natural dyes reemerged as a potential viable Green chemistry option as an
alternative/co-partner to some extent to synthetic dyes (Yusuf
et al., 2011; Mirjalili et al., 2011). Recent resurgence in research
and development on natural dye production and application is
observed due to increasing popularity of more natural lifestyle
based on naturally sustainable goods (Grifoni et al., 2009). Natural
ora/fauna is full of exquisite colors fascinating and attracting
* Corresponding author. Tel.: 91 9350114878.

E-mail addresses: mshahid96@gmail.com (M. Shahid), shads.jmi@gmail.com
( Shahid-ul-Islam), faqeermohammad@rediffmail.com (F. Mohammad).
0959-6526/$ e see front matter ! 2013 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.jclepro.2013.03.031
human being towards a vast portfolio of possibilities (Dawson,

2009). A large number of plant and animal/insect sources have
been identied for extraction of color (Guinot et al., 2006; Kumar
and Sinha, 2004) and their diversied use in textile dyeing
(Samanta and Agarwal, 2009) and functional nishing (Gupta et al.,
2005), food coloration (Delgado-Vargas et al., 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 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 dyes in functional nishing 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 dyes a
viable co-partner/alternative to synthetic dyes.
2. Technological advancements in textile coloration with

natural dyes
Coloration is an integral part of ever expanding complex
chemical wet processing of textiles, which involves use of many
types of chemical entities and physico-chemical processes.
M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331
311
Fig. 1. Various applications of natural dyes.
Environmental concerns arising due to accelerated development in

textile wet processing industry paved the way for ongoing interest
in the development of cleaner production strategies for making
cost-effective value added textile products (Ahmed and ElShishtawy, 2010).
Hill (1997), while discussing lack of quality research work on
natural dyeing techniques 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 15 years,
investigations 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
information on natural dyeing techniques are available today.
Natural dyeing in textiles is currently of great interest in both
research elds as well as textile industries due to increasing attention to the aspects of water pollution, sustainability of raw materials
and processed products, biodegradability and environment-friendly
attributes (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 as ultrasonic
(Kamel et al., 2005), microwave (Nourmohammadian and Gholami,
2008), pad dyeing (Mongkholrattanasit et al., 2010; Ratnapandian
et al., 2012), High Temperature High 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 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 Saikia, 2005; Sharma et al., 2012a), processing
improvement for natural colorant extraction (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 of natural dyeing methods and use of
modern day technologies in different stages of natural 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 techniques and the overall process must be competitive with regard to the use of chemicals, energy,
wastes and wastewater and overall costs (Bechtold and MahmudAli, 2008).
2.1. Mordants and mordanting
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 mainly focused on
the use of mordants. In addition to creating afnity between dye
and bre, the use of mordants also change the hue of certain dyes.
Different mordants used with the same dye may darken, brighten
or drastically alter the nal color of the dyed bre (Manhita et al.,
2011; Yi and Cho, 2008). Colorimetric properties of the dyed fabrics such as Lightness (L*), redness-yellowness (a*), bluenessgreenness (b*), chroma (c*), hue (ho) and color strength (K/S) are
greatly dependent on the chemical nature of mordants and bres
and the metal ion complex forming ability with the dye and the
bre (Tang et al., 2010). Mordanting generally improved dye performance and help the dyer to achieve a broad spectrum of colors
on a wide range of natural as well as synthetic bres with expanded
312
Table 1
List of metallic mordants used in natural textile dyeing.
Mordants
Chemical formula
References
Conventional metallic mordants

Alum
Ferrous sulphate
Stannous chloride
Copper sulfate
Potassium dichromate
KAl(SO4)2$12H2O
FeSO4$7H2O
SnCl2$2H2O
CuSO4$5H2O
K2Cr2O7
Park et al., 2005; Samanta and Agarwal, 2009;Vankar et al.,

2007a, 2008a; Zarkogianni et al., 2011
MgSO4$7H2O
Al2(SO4)3
ZnSO4$7H2O
MnSO4$5H2O
NiSO4$6H2O
CoSO4$6H2O
SnSO4
SnCl4$5H2O
FeCl3
CuCl2$2H2O
ZnCl2
AlCl3$6H2O
Al(NO3)3$9H2O
Ca(OH)2
Zn(BF4)2
La2O3
Das et al., 2008; Moiz et al., 2010;Rekaby et al., 2009

Das et al., 2008; Hwang et al., 2008;Yi and Cho, 2008
Ghouila et al., 2012; Guesmi et al., 2012a,b;Onal et al., 2005
Hwang et al., 2008; Lee and Kim, 2004
Hwang et al., 2008; Lee and Kim, 2004
Guesmi et al., 2012a,b; Hwang et al., 2008;
Hwang et al., 2008
Vankar et al., 2007a, 2008a
Mikropoulou et al., 2009; Rekaby et al., 2009;Zarkogianni et al., 2011
Ibrahim et al., 2010
Ibrahim et al., 2010; Zarkogianni et al., 2011
Onal et al., 2005
Chairat et al., 2007
Wang et al., 2012
ReCl3$6H2O
NdCl3$6H2O
ZrOCl2$8H2O
Zheng et al., 2011

Zheng et al., 2011
Newly discovered metallic mordants

Magnesium sulphate
Aluminium sulphate
Zinc sulphate
Manganese sulphate
Nickel sulphate
Cobalt sulphate
Stannous sulphate
Stannic chloride
Ferric chloride
Copper chloride
Zinc chloride
Aluminum chloride
Aluminium nitrate
Calcium hydroxide
Zinc tetrauoroborate
Lanthanum oxide
Rare earth chlorides
Rhenium trichloride
Neodymium trichloride
Zirconium oxy chloride
shade ranges and better fastness properties (Kadolph and

Casselman, 2004). Samanta and Agarwal (2009) presented a
comprehensive review of studies available on different types of
mordants, mordanting methods and their effects on natural dyeing
for a variety of textile materials. Most commonly used mordants in
natural dyeing are aluminium potassium sulphate, potassium dichromate, stannous chloride, ferrous sulphate and copper sulphate
(Samanta and Agarwal, 2009). Improving traditional mordanting
processes and selecting new mordants to replace traditional heavymetal 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 (Table 1).
Zheng et al. (2011) have successfully employed rare earth chlorides
as mordant for 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 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.
Natural dyeing processes typically generate wastewater containing residual toxic metal ions 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 products and efuent discharged from textile
industries is strictly prohibited beyond a certain specied limit.
Alum and ferrous sulphate are considered safest among metallic
salt mordants and tin can be used up to certain limits while use of
chrome and copper is almost banished considering their toxic nature (Savvidis et al., 2013; Zarkogianni et al., 2011). While dyeing
with natural dyes, a substantial proportion of mordant remains
unexhausted in the residual dyebath and thus may pose serious
efuent problems, hence, it is important to pay special attention to
the limit values of metal ions in textiles and efuents prescribed by
Environmental Protection Regulations.
Considering above environmental concerns, use of natural
mordants (Table 2) in place of 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 with high tannin
content (Prabhu and Teli, 2011) or metal hyperaccumulating plants
(Cunningham et al., 2011). Recently chlorophyll extracted from
different plant sources has also been successfully employed as
biomordant (Guesmi et al., 2012a,b). Vegetable tannins are water
soluble polyphenolic compounds found in wide variety of plant
parts such as bark wood, fruit, fruit pods, leaves, roots and plant
Table 2
List of plants used as source of biomordants in natural textile dyeing.
Botanical Name
Reason for use as

mordant
References
Acacia catechu
Used as sources
Emblica ofcinalis
of tannin mordant
Entada spiralis
Eucalyptus
Memecylon scutellatum
Punica granatum
Quercus infectoria
Rhus coriaria
Rumex Hymenosepolus
Tamarindus indica
Terminalia bellerica
Terminalia chebula
Prosopis spp.
Enterolobium
cyclocarpum
Caesalpinia coriaria
Mansour and Heffernan, 2011

Prabhu et al., 2011
Sachan and Kapoor, 2007
Chattopadhyay et al., 2013
Grifoni et al., 2011
Bruni et al., 2011
Haji, 2010
Prabhu and Teli, 2011
Shekhawat, 2012
Samanta et al., 2011
Shekhawat, 2012
Arroyo-Figueroa et al., 2011
Symplococcus sp.
Aporusa sp.
Baccaurea racemosa
Xanthophyllum
lanceatum
Eurya acuminata
Al-hyperaccumulating
plants used as
substitute of alum
mordant
Cunningham
Cunningham
Cunningham
Cunningham
Pyrus pashia
Cu rich plant used as

substitute of copper
mordant
Arroyo-Figueroa et al., 2011

et
et
et
et
al.,
al.,
al.,
al.,
2011
2011
2011
2011
Vankar et al., 2008d

Vankar and Shanker, 2009
313
galls. Phenolic hydroxyl groups of tannins enable them to form

effective crosslinks with different types of bres and dyes and help
in color xation. Tannin based mordants were found most effective
in case of cotton bre which has very low afnity for most of the
natural dyes (Prabhu and Teli, 2011).
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 of
traditional Indonesian textiles and its impact on religious, social
and economic scenario. They emphasized on the prerequisite of
knowledge of chemistry, cultural requirements and resource
management for effective utilization of several other possible
sources of Al-hyperaccumulating plants in addition to traditionally
used plants. Recently Vankar et al. (2008d) observed that Euriya
acuminata when used as mordant in conjunction with Rubia cordifolia dye was found to enhance the dyeability of silk fabric by
chelation due to the high 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 avone/avonol dyes extracted from Delonix
regia (Vankar and Shanker, 2009). Use of metal hyperaccumulating
plants as natural source of metal mordants is very promising
concept which should be popularized as an alternate method that
may help to reduce the reliance on toxic metal salt mordants.
2.2. Enzyme assisted dyeing
The use of enzymes in textile industry is an example of industrial biotechnology, which allows the development of environment-friendly technologies in bre processing and strategies to
improve the quality of nal product. Different types of enzymes are
commonly used in various stages of textile processing for modication of physical and chemical surface properties or introduction
of functional groups on the surface of textile bres (Duran and
Duran, 2000; Jo et al., 2008). Many different approaches have
been taken to the preparation, dyeing and nishing of cotton
(Vankar and Shanker, 2008), wool (Montazer et al., 2009), silk
(Vankar et al., 2007b; Vankar and Shanker, 2009) and other textile
bres (Sricharussin et al., 2009) with natural colorants using
different types of enzymes. Tsatsaroni and co-authors used aamylase, amyloglycosidase and trypsin enzymes for preparation of
cotton and wool samples for dyeing with saffron and curcumin
(Kyriakides et al., 1998; Tsatsaroni et al., 1998). They 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 bres. Kumbasar et al. (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 and gallnut and reported signicant increase in dye uptake after enzymatic treatment. 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, diasterase, proteaseeamylase on dyeing characteristics of Terminalia arjuna, Punica granatum, Rheum emodi (Vankar
et al., 2007b), Acacia catechu, Tectona grandis and 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 improvement by enzymatic treatment. They showed that dye enzyme
compatibility is an important factor in enhancing dyeing properties: proteaseeamylase combination is suited for Acacia and Terminalia; lipase is suited for Rheum and Delonix, while diasterase is
suited for Tectona and Punica. Compared to untreated wool, treatments with protease and transglutaminase enhanced K/S value of
wool dyed with sappan dye; however, no signicant changes were
observed in fastness characteristics (Zhang and Cai, 2011).
Although studies of enzymes used in natural textile dyeing
(Table 3) have received limited attention in scientic literature,
however, from the point of view of processing improvement,
quality enhancement of processed products, increased resource
consumption and reduced environmental impacts by enzymatic
dyeing induced the search for more industrial enzymes. The latest
development concerning advances in enzymatic application techniques provide possibilities for the development of new enzymebased natural dyeing systems for a more 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 adopt enzyme assisted dyeing method
on commercial scale.
2.3. Sonicator-assisted dyeing
The application of ultrasound power to textile dyeing has a
signicant role in the concept of clean technology for textile
Table 3
Enzymatic application in natural Textile dyeing.
Reference
Enzyme
Substrate
Class
Trade name
Source
Raja and Thilagavathi, 2011
Protease
Zhang and Cai, 2011
Protease
Transglutaminase
Laccase
Protease
Protease
Savinase 16L
e
Denilite II S
Novolan T
Savinase
e
e
e
Bacillus sp.
Bacillus
licheniformis
Bacillus
amyloliquefaciens
Aspergillus oryzae
Aspergillus niger
A. niger
e
e
e
Montazer et al., 2009

Parvinzadeh, 2007
Kumbasar et al., 2009
Alcalase
Vankar et al., 2006;
Vankar and Shanker,
2008,2009
Kyriakides et al., 1998;
Tsatsaroni et al., 1998
e Not specied.
Protease
Amylase
Lipase
Diasterase
Amylase
Trypsin
e
e
e
e
e
e
Treatment conditions
pH
Temp.
(" C)
Treatment
time (min)
Wool
70
60
Wool
8
7
4.5
7
9e9.5
50
50
60
30
50
45
40
60
60
20
8e8.5
60
20
7.2
7.1
7.0
7.2
7
8
25
30
30
25
e
e
10
10
10
10
10
30
Wool
Wool
Wool
and silk
Cotton
and silk
Cotton
and wool
Natural dyes used in the study
Grevillea robusta, Spathodea campnulata,

Cassia auriculata, Acacia decurrens
Caesalpinia sappan
Rubia tinctorum
Rubia tinctorum
Rhus coriaria, Terminalia chebula, Quercus
alba, Quercus infactoria
Terminalia Arjuna, Punica granatum, Rheum

emodi, Acacia catechu, Tectona grandis,
Delonix regia
Crocus sativus, Curcuma longa
314
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 implosive collapse of small gas bubbles caused by ultrasonically induced alternating compression and rarefaction
waves. The cavitation bubbles oscillate and implode, thus
enhancing molecular motion and stirring effect in the dyebath.
When cavitation occurs at a solid/liquid interface (e.g., a bre/
dyebath interface), the resulting asymmetric implosion produces
micro streaming towards the solid surface which greatly disrupts
the diffusion interlayer and promotes mass transport in that direction (Vankar et al., 2008a,b). Cavitation and its physico-chemical
consequences enhance the dyeing rate; economize energy and time
consumption without causing any apparent bre damage (Vankar
and Shanker, 2008). In the last few years a certain number of
studies on ultrasound assisted natural dyeing and nishing of
natural and synthetic bres were carried out at the experimental
level. Ultrasonic energy provided easy efcient route for dye
extraction, mordanting, and dyeing processes in comparison with
the traditional methods (Mansour and Heffernan, 2011).
Kamel et al. (2005, 2007, 2009a, 2009b) comparatively investigated various parameters for 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) extractability and dyeability of bres in
comparison with conventional heating as a result of ultrasonic
cavitation effect. Vankar and coworkers discussed the effectiveness of ultrasound technology for dyeing of different type of
textile bres with commercially available natural dyes such as
catechu, tectona (Vankar and Shanker, 2008), madder (Vankar
et al., 2008d) and identication, extraction and application of
natural dyes from new vegetable sources such as Ixora coccinea
(Vankar and Shanker, 2006), Eclipta alba (Vankar et al., 2007a),
Symplocos spicata (Vankar et al., 2008a), Acer pectinatum (Vankar
et al., 2008b), Mahonia napaulensis (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 dyeing in terms
of enhanced resource productivity, reduced wastes, reduced
concentration of dyes and electrolytes in dyeing-bath and efuent
along with signicant 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 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 (Mansour and Heffernan,
2011) is found to have a signicant improvement in dye uptake
representing sonication efciency in textile dyeing. Sivakumar
et al. (2009, 2011) studied extraction of colorants from some
dye yielding plants such as beetroots, Green wattle barks, Marigold owers, Pomegranate rinds, 4O clock plant owers and
Cocks comb owers and reported signicant improvement in
extraction efciency of the colorants due to the use of ultrasound.
Guesmi et al. (2013) reported substantial improvement of about
49.62% more dye uptake in case of sonicator dyeing of modied
acrylic fabrics with indicaxanthin natural dye in addition to better
light, washing and water fastness results than the conventional
method.
The use of ultrasonics in natural textile dyeing provides the
following benets:
# Energy savings by dyeing at lower temperatures and reduced

processing times,
# Reduces pollution load by reduced consumption of auxiliary
chemicals and increased dye exhaustion levels,
# Improves processing efciency and yield better product quality
by allowing real-time control of color shade,
# Minimize damage to bres during dyeing,
# Lowers overall processing costs, thereby increasing industry
competitiveness.
Use of sonication method for textile dyeing on commercial scale
is denitely a cleaner production strategy that offers an environmentally benign alternative to traditional exhaustion method. As a
general conclusion it could be said that replacing conventional
thermal dyeing method with sonication method could make the
process highly efcient, energy saving, economical and low waste
generation technique.
2.4. Other chemical and radiation pre- and post-treatments
Recent developments in natural textile dyeing mainly rely on
the modication of natural and synthetic bres using various preand post-treatment agents for improvement in color, fastness and
functional characteristics of dyed fabrics along with the focus on
environmental compatibility of these modication methods. Effect
of various surface modication agents 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 natural dyes have been evaluated
frequently. Results indicated that pre-treatment of different types
of fabrics with cationic and anionic agents enhances color strength
and fastness properties of dyeings over untreated dyeings to a
signicant extent. Fibre surface modication by the use of synthetic
and natural polymers is also employed successfully for enhancing
absorption capacity naturally dyed bres (Janhom et al., 2004,
2006). In recent years, a number of investigations have been carried
out to exploit potential applicability of chitosan, a naturally
occurring biopolymer with distinct chemical and biological properties, as surface modication agent to improve dyeing performance and biofunctionalisation of 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 dye absorption (Chairat et al., 2011).
Recently, dry modication processes such as sputtering and
low-temperature plasma (LPT) treatment techniques that generate
no waste have been introduced for the pre-treatment and nishing
of textile fabrics as environment-friendly alternative to wet
chemical applications (Ghoranneviss et al., 2011; Shahidi and
Ghoranneviss, 2011). Plasma treatment of bres improves surface
characteristics of bres while the bulk properties of the bres are
not affected (Barani and Maleki, 2011). Wakida et al. (1998) marked
the associated benets of oxygen, carbon tetrauoride, 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-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 showed that pre-treatment of PET
fabrics with chitosan and/or plasma is better than a metal 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 brous surfaces
yielding hydrophilic species, thereby increasing dyeing afnity
with curcumin natural dye (Kerkeni et al., 2012). Chemical
modication of cotton fabric with reactive cyclodextrin (R-CD) at

different concentrations resulted in remarkable enhancement in
printability of cotton fabric as well as color strength of printed
sample; however there was no remarkable difference between
fastness properties of modied and unmodied samples (Hebeish
et al., 2006).
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 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 prepared as a means
of improving the light fastness of naturally dyed fabrics provide a
novel 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).
Hydrophobic acrylic bres pose a big problem for dyers due to
their hydrophobic nature. Incorporation of amino groups to acrylic
fabrics by treatment with hydroxylamine hydrochloride is reported
to increase substantively of the bre towards some anionic natural
dyes (Guesmi et al., 2012a, 2013). Modied acrylic bre containing
different amounts of amidoxime groups showed better dye uptake
along with signicant improvement in color characteristics (ElShishtawy et al., 2009). Considering pH sensitivity of natural dyes
some researchers implied ammonia after treatment as useful
technique to obtain better shades with improved colorimetric
properties (Montazer et al., 2004; Montazer and Parvinzadeh,
2004). The preliminary studies on natural dyeesurfactant interactions have shown that dyeing of bres with the natural dyes in
the presence of the surfactants enables good shade and fastness in
color at low temperatures to be achieved and may minimize the
damage to bres during dyeings (Chandravanshi and Upadhyay,
2012). Use of high energy radiations such as UV (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 benecial in improving the dye uptake and color characteristics of naturally dyed fabrics.
Pre-treatment and nishing of textile fabrics by modern surface
modication techniques, such as use of eco-friendly biopolymers,
plasma and radiation treatment technologies, relate to environmentally clean textile processing methodology and are much superior to traditional chemical modication methods. Increasing
momentum of advanced technologies in sustaining green chemistry aspects of processing and application shows that there is a
signicant potential to reduce the ecological impact of existing
processes with the introduction of these new concepts in real-time
methodologies of textile dyeing and nishing focusing on realizing
higher productivity gains in consumption of natural dyes without
compromising with eco-safety standards.
2.5. Environmental and socio-economic sustainability aspects of
natural textile dyeing
In recent years, both researchers and practitioners have devoted
attention to environmental and socio-economic sustainability issues in the textile industry (Thiry, 2011; Caniato et al., 2012).
Despite the industrial relevance of the issue, structured analysis of
the perspectives 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 natural dyes in modern textile industry. Since natural dyeing
does not exist on a commercial scale in modern textile industry,
315
currently most of the studies are based on laboratory results or

model processes. However, some discrete group of researchers
have investigated the ecological position, future demands and
availability of raw material, the handling, products properties,
renewability and standardization for large scale production of
natural dyes, leveraging on environmental and economic sustainability to reach out to new market niches (Bechtold et al., 2003;
Bechtold and Mahmud-Ali, 2008).
Basically, main sources of natural dyes can be divided in three
categories:
1. Primary products from agriculture
2. Waste and byproducts from farming and forestry
3. Wastes from the food and beverage industries
Most of these studies available on natural dye sources and
dyestuff extraction centered on collecting plant materials from wild
and exploring the coloring properties of extracts from different
plant parts. However, direct commercial use of native plants in
dyestuff production without investigating sustainability issues
seems impractical and will lead to overexploitation of natural resources. Studies focusing on agronomic potential and related
environmental consequences critical to harvesting natural dye
yielding crops are rare. Indigo, madder, and weld are some wellscreened natural dye crops which can be protably harvested for
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 et al., 2003; Siva,
2007). Standardized collection of this type of 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 rst step in assuring environmental and socio-economic
reality. Furthermore, for the commercial exploitation, the selected
species must also be screened for their appropriateness in purview
of modern sustainable cultivation techniques.
It is well known that the industrial system is very wasteful of
materials and recycles very little (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 the fulllment 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
organism leads to the idea that some industry can always be found
to consume another industrys wastes, although not always true, is
very reasonable in natural dye production from industrial wastes.
Use of cheap byproducts from agriculture and forestry such as bark
from timber industry e.g. Ash tree bark (Bechtold et al., 2007a), and
leaves from abundantly available plants such as teak (Prusty et al.,
2010), eucalyptus (Mongkholrattanasit et al., 2010), is a promising
concept which can lower costs involved in natural dye production.
Industrial food and beverage production produces huge amount of
colored plant wastes such as pressed berries and distillation residues (Bechtold et al., 2006), pomace (Bechtold et al., 2007b), peels
(Sinha et al., 2012), shell (Ismal and Yildirim, 2012), and other residual byproducts (Meksii et al., 2012) containing considerable
quantities of coloring matters which can be utilized as promising
source of natural dyes for textile industries after some careful
investigation of supply chain system and optimization of processing
variables (Bechtold and Mahmud-Ali, 2008; Bechtold et al., 2009).
Olive mill wastewater (OMW) (a byproduct of olive extraction industry responsible for serious environmental concerns in Mediterranean countries, as around 30 million m3 of OMW produced
annually in this region) can be used as prospective source of natural
316
coloring substances in olive oil producing countries which are

renewable, available in high quantities and free costs (Meksi et al.,
2012). An intensied use of industrial waste as renewable raw
material for natural dye production represent sustainable cleaner
production strategy as in addition to minimizing waste production
and conservation of fossil fuels, it would maximize economical use
of waste materials.
Production cost of natural dyes from direct harvesting are high
as compared to production costs from waste and byproducts.
However, colors provided by agricultural primary production could
not be obtained with residues. Thus, any industrial natural dye
production unit must include both direct agricultural as well as
residual sources for obtaining a complete color palette. Strategic
combination of different plant sources allows the minimization of
cost to certain extent, and the average production cost of total
color portfolio could be within 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 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 wastewater and plant residue, which require complicated
aftertreatments leading to additional costs from 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: rstly, it increases cost of
dyeing process as unxed dye is not available for the coloration
process and secondly, the dye present in the wastewater has to be
removed in order to fulll legal limits for textile efuents (Mussak
and Bechtold, 2009).
Use of sonication in extraction and dyeing process presents a
probable alternative to traditional thermal exhaustion method of
natural dyeing, as it increases dye exhaustion to a greater extent
thus decrease the efuent load and cost of natural dyeing
(Sivakumar et al., 2009; Mansour and Heffernan, 2011). Research
ndings on using enzyme as fabric pre-treatment method offers a
cost-effective and environmentally favorable soft chemistry option as enzymes are specic and fast in action and small amounts of
enzyme often save large amounts of raw materials, chemicals, energy and water (Vankar and Shanker, 2008; Montazer et al., 2009).
Another interesting aspect is reusing spent dye liquor in repeated
dyeing cycles (Vankar et al., 2007b). Economic analysis as done by
Shams-Nateri (2011) on reusing wastewater for wool dyeing with
madder caused 19.91% cost saving.
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 natural dye
extraction creates an additional burden of waste disposal. Vankar
et al. (2011) presented a very interesting study on biosorption efcacy of waste pulp generated after natural dye extraction from
some selected biomaterials (Canna indica ower, Portulaca olecera
ower and stem, Hibiscus rosasinensis ower and Trapa natans fruit
skin) as an alternative use other than just composting it. They
demonstrated that use of natural dye waste as heavy-metal adsorbents can be very effective in remediation of groundwater and
surface water of chrome metals in contaminated sites of tannery
operations.
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 (Fig. 2), the use of natural colorants
is expected to contribute to sustainable development in the near

future (Ganglberger, 2009).
3. Natural dyes in functional nishing of textiles
The role of the textile nisher has become increasingly
demanding, and now requires a careful balance between compatibility of different nishing products and treatments and the
application processes used to provide textiles with desirable
properties. Consumers worldwide are looking for clothing and
other textile products which provide greater comfort and remain
fresh, hygienic and odor free in use. Investigation for innovative
methods, for development of hygienic textile products, in textile
nishing processes and existing applications and problems in this
area is the need of the hour. A number of reports are now 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 al., 2008; Lee et al., 2008)
and UV-protective (Sarkar, 2004) properties. Chemical constituents
of some important natural dyes used in functional nishing of
textiles are given in Fig. 3.
3.1. Antimicrobial nishing
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 textiles
during use and storage imposes a number of undesirable effects for
the textiles as 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 organometallics, phenols, organo silicones, quaternary
ammonium compounds, N-halamines, chitosan, polybiguanides,
triclosan, nanoparticles of noble metals and metal oxides, and
bioactive plant-based products (Gao and Cranston, 2008; Simoncic
and Tomsic, 2010). Most of them are complex in nature and take
long time to complete their natural cycles and return to nature. The
challenges faced by textile nishing industry have intensied
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
nishing agents for making textile products that can offer improved
protection to the users from microbes (bacteria, mould or fungi) by
preventing the growth of microorganisms on fabrics used in wide
range of clothing, home furnishings, commercial and industrial
products (Gupta and Bhaumik, 2007; Ramchandran et al., 2004).
With the steady increase in number of safe and durable antimicrobial agents and textile nishing techniques, bioactive textiles are
easily nding a place in the global textile market. Recent developments in bioactive agents of 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 known and
some of these have been shown to posses signicant 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
owing to the existence of tannins (Prabhu and Teli, 2011; Shahid
et al., 2012), avonoids (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-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).
Gupta and coworkers have studied antimicrobial properties
of eleven commercially available natural dyes against some
317

ENERGY
WATER
FERTILIZER
PESTICIDES
CULTIVATION
e.g. Indigo, Madder,

Weld, Sawwort
CROP
WASTE = LEAVES
e.g. Teak, Eucalyptus
WASTE
e.g. Pressed berries, Pomegranate peel,
Onion peel, walnut husk,
Olive mill waste water
TIMBER INDUSTRY
WASTE
WASTE = BARK
e.g. Ash tree bark, Alder,
can
be
utilized as
Animal feed
Soil conditioner
Adsorbent
FOOD INDUSTRY
FORESTRY
FOOD &
BEVERAGES
WOOD
ENERGY
AND
SOLVENT
EXTRACTION AND STANDERDIZATION
WASTE
can be utilized as
DYESTUFF
ENERGY
WATER
DYEING AUXILARIES
DYEING PROCESS
Waste Compost
Waste Biofuel
Adsorbent
WASTE WATER
Reuse of spent
dye liquor for
lighter shades
WASTE WATER CONTAINING

MINIMUM CHEMICAL LOAD
(Released to wastewater
treatment plant)
DYED TEXTILES
Fig. 2. A schematic representation of enhanced resourse utilization and waste minimization in a natural textile dyeing.
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 present in solution form
than when it is held intimately to the textile substrate. Han and
Yang (2005) studied antimicrobial effect of curcumin (a yellow
orescent pigment of carotenoid 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 these relations, antimicrobial activity of
wool fabrics nished with curcumin can be predicted on the strains
of Staphylococcus aureus and Escherichia coli without antimicrobial
testing. Berberine, a natural cationic colorant was successfully
employed onto cotton (Kim and Son, 2005), wool (Ke et 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 curcumin each separately as well as
in different combinations to impart antimicrobial activity 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 corresponding intact ones.
Antimicrobial tests conducted on natural dyes obtained from
different plant waste materials such as waste leaves and supercial
barks of Terminalia catappa, Artocarpus heterophyllus, Tectona
grandis, Morinda citrifolia (Prusty et al., 2010), Albizia lebbek and

Saraca asoca (Baliarsingh et al., 2012) demonstrate an exciting opportunity for producing naturally dyed silk yarn as a potential
sustainable technique towards waste utilization and development
of protective clothing. Ibrahim et al. (2010) investigated various
factors affecting dyeing and multifunctional properties of knitted
cotton fabric such as fabric structure, type and concentration of
mordants, kind and percent of 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
Gve > G$ve; most probably due to the fact that Gve bacterial
cell wall consists of a single layer whereas G$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 A. catechu (Khan et al., 2011),
Lawsonia inermis (Yusuf et al., 2011, 2012), R. 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 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 can be
applied as antimicrobial nishing agents on silk (Saranya et al.,
2012), cotton and 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
318
Turmeric (Curcuma longa)

O
Indian Rhubarb (Rheum emodi)

OH
R1
OH
R2
OH
HO
R1
R1 =OCH3, R2 = OCH3 Curcumin

R1 =OCH3, R2 =H
Demethoxycurcumin
R1 =R2 =H
Bisdemethoxycurcumin
Weld (Reseda luteola)
R1=H, R2=CH3 Chrysophanol; R1=H, R2=CH2OH Aloe-emodin

R1=H, R2=COOH Rhein; R1=CH3, R2=OH Emodin;
R1=CH3, R2=OCH3 Physcion
Eucalyptus (Eucalyptus globulus)

OH
Cutch (Acacia catechu)
OH
OH
HO
R2
HO
OH
HO
OH
OH
OH
R= OH Luteolin
R= H
Apigenin
Flos sophorae (Sophora japonica)

OH
OH
HO
Catechin
R= OH Quercetin
R= OC12H22O9 Rutin
Onion (Alium cepa)

OH
OH
OH
Gallnut (Quercus infectoria) &

Pomegranate (Punica granatum)
OH
COOH
OH
HO
HO
OH
OH
OH
Quercetin
Indigo (Indigofera tinctoria)

O
OH
HO
OC H O
12 22 9
Gallic acid
Gromwell (Lithospermum
erythrorhizon)
Ellagic acid
O
N
Indigo
OH
Cochineal (Dacylopius coccus)

OH
HO
OCH 3
CH3
Jackfruit (Artocarpus heterophyllus)

HO
OCH 3
Berberine
Shikonin
Teak (Tectona grandis)

R1
OH
OH
R3
HO
COOH
OH
OH
OH
OH
HO
CH3
HO
Berberry (Berberis aristata)
OH
HO
OH
Rutin
OH
OH
CH3
OH
OH
Morol
Carminic acid
Madder (Rubia tinctorum & Rubia cordifolia)

O
R1
R2
OH
R1=H, R2=H, R3=COOH Tectoquinone

R1=OH, R2=OH, R3=CH3 Tectoleafquinone
Henna (Lawsonia inermis)
R2
O
OH
R4
R3
R1=OH, R2=OH, R3=H, R4=H

Alizarin;
R 1=OH, R2=OH, R3=H, R4=OH Purpurin
R1=OH, R2=COOH, R3=OH, R4=OH Pseudopurpurin; R1=OH, R2=CH3, R3=OH, R4=H Rubiadin
R1=H, R2=OH, R3=COOH, R4=OH Manjistin
R 1=H, R2=OH, R3=H, R4=OH Xanthopurpurin
Fig. 3. Chemical structures of the main constituents of the natural dyes used in functional nishing of textiles.
Lawsone
(Prabhu et al., 2011; Prabhu and Teli, 2011). Few recent reports
pointed out the use of 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, 2011), cationization (Hong et al., 2012), microencapsulation and cross-linking (Sathiyanarayanan et al., 2010) methods
for enhancement in antimicrobial activity of naturally dyed textile
materials. These innovative methods proved of immense help in
improving bioactive properties of nished products.
Although, several efforts have been made to exploit various
natural dyes for antimicrobial nishing of textiles, but still there is
scarcity of systematic and logical approach for implementation of
these ndings in real market of protective antimicrobial textiles.
There are several key issues which are still remaining to be looked
into. The major challenge in establishment of natural dyes as textile
antimicrobial agents is the procurement of these products in bulk
quantities; and standardization of their extraction, purication and
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.
Durability of nishing is a major concern to textile researcher
and users since the nished 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 ndings reported in
cited literature demonstrate an exciting opportunity for the naturally dyed textile as a potential perspective in developing protective
clothing and other textile products for various application elds.
3.2. UV-protective nishing
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 changes such
as excessive exposure to sunlight during leisure activities have increase chances of skin cancer. Exposure to the sun is an occupational
hazard to outdoor workers such as construction industry workers,
recreation workers, sportspersons, agricultural and horticultural
workers, and shermen as they have no choice about the duration of
their exposure to sunlight. This necessitates the development of UVprotective clothing and coverings to minimize the effect of harmful
Ultraviolet radiation. UVR transmission properties of textiles are
inuence by many factors such as structure and physiochemical
nature of bre, dyes and nishes, fabric thickness, porosity and
moisture content (Gies, 2007; 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, delustrants, or ultraviolet absorber nish is present that
absorbs ultraviolet radiation and 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 and Crews, 2005).
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) 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.
Feng et al. (2007) in an experiment conducted to evaluate UV
protection properties of two natural dyes (Rheum and Lithospermum erythrorhizon) applied on cotton and silk found that
these natural dyes exhibit a comparable UV-absorption performance to benzophenone. Results demonstrated that UV-protective
effect was strongly dependent on absorption characteristics of
319
natural dyes for UVR. Grifoni et al. (2009, 2011) studied the effect of
color on UVR transmission of cotton, ax, hemp and ramie fabrics
with different construction parameters dyed with some common
natural dyes by in vitro and outdoor assessments. The 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 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 properties of naturally dyed cotton (Gupta
et al., 2005), wool (Mongkholrattanasit et al., 2011a) and silk
(Mongkholrattanasit et al., 2011b; Wang et al., 2009) fabrics to a
substantial account depending on nature of bre, mordant and
natural dye used. Very recently, Hou et al. (2013) used natural dyes
extracted from orange peel (OP), an abundant, cheap and readily
available agricultural byproduct, for producing highly durable UVprotective wool fabrics. They reported that UPF value of OP treated
wool fabric was six times higher than that of the 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 higher than wool dyed with synthetic
dyes.
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 primary tool in
shielding UV radiations. Measurements of their properties in
blocking UV 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 environmental and energy conservation benets, in developing high
performance materials for the world market. Therefore, it is
contemporary need to develop a proper treatment to increase the
UV protection property to fabrics. Promising research ndings obtained from laboratory scale and outdoor experiments shows that
naturally dyed fabrics with UV-protective properties seem to have
bright future after some rigorous research and development.
3.3. Insect repellent nishing
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 signicant economic
losses, especially in warehouses and showrooms. Even a small
amount of bre eaten from a valuable suit or a rug can ruin its
functional and/or aesthetic properties. Insect repellents that
discourage insect damage in textile industry are in great demand.
Kato et al. (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 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, indigo,
Amur cork tree extract. Park et al. (2005) studied in detail the insect
resistance of eight naturally occurring quinones and avonoid dyes
after application to wool with ve 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 insect deterrence
against black carpet beetles.
4. Natural dyes in dye-sensitized solar cells (DSSCs)
At present, we are mostly dependant on fossil fuels i.e. coal,
crude oil and natural gas for our energy needs. These fuels being
320
non-renewable and limited in supply are constantly exhausted,

thus are creating a huge problem for the future generations.
Therefore, a search for renewable low environmental impact
alternative energy sources is considered one of the top priorities in
todays society. Among renewable energy resources, solar energy is
the largest exploitable resource, which provides more energy in 1 h
to the earth than all of the energy 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 conversion of visible light into electric
energy which provides a technically and economically credible
alternative concept to present day pen junction photovoltaic devices (Gratzel, 2003).
It has emerged as one of the promising renewable energy
sources for eco-friendly and cost-effective conversion of solar energy to electricity and due to the use of inexpensive materials,
simple fabrication process and low environmental impact, especially those sensitized by 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 cells can work effectively in low light conditions and
are less susceptible to losing energy to heat. The efciency of DSSC
is determined mainly by the sensitizer used. The dye as a sensitizer
plays a key role in absorbing sunlight and transforming solar energy into electrical energy (Zhou et al., 2011). DSSCs with efciencies 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 (Campbell et al., 2007).
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 reports have
emphasized on exploration into natural dyes, such as cyanine
(Sirimanne et al., 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; 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 alternative for use in dye-sensitized solar cells.
Although these natural dyes often work poorly in DSSCs, these are
expected as low cost and prepared easily comparing to ruthenium
(Ru) complex based dyes.
Different types of natural dyes showed different solar conversion efciencies depending on 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 et al.,
2011; Zhou et al., 2011). Natural dye-sensitized DSSCs usually
perform poorly in DSSC because of weak binding energy with the
metal oxide lm (photo-electrode) and low charge-transfer absorption in the whole visible range. Based on investigation on the
structure and properties 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 on and the TiO2 lm on cathode in DSSCs. Heera and
Cindrella (2010) theoretically evaluated ten natural pigments: caffeic acid, ferulic acid, ellagic acid, deoxysantalin, resveratrol (plant
source), carminic acid, kersemic acid, ommatin D (insects),
methoxatin and 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 efcient application in DSSC due to their favorable
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
TiO2 and ZnO substrates and conrmed that the efciencies obtained with TiO2 are much higher than for ZnO substrates, in
Fig. 4. Schematic representation of working of dye-sensitized solar cells.
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 surface of
TiO2 lm 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. Extracting temperature,
extracting solvent and pH of the extract solution also have very
prominent role in determining efciency and stability of DSSCs
(Chang et al., 2010; Wongcharee et al., 2007).
Meng et al. (2008) elucidated the electronic coupling between a
TiO2 nanowire and a cyanidin natural dye sensitizer and provided
insight into charge injection mechanisms of natural dye-sensitized
nanowire solar cells. By exploring various nanowire orientations
and 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 components,
and improved light scattering and charge transport, all of which
contribute towards improving key characteristics, that is, low cost
and high efciency. DFT characterization of the molecular properties
of different natural pigments relevant to dye-sensitized solar cells
for better understanding of the electron injection process is also
reported in literature (Qin and Clark, 2007; Sang-aroon et al., 2012).
Several innovative methods have been developed for performance improvement of natural dye-sensitized solar cells. The
incorporation of carbon nanotubes as counter electrode in natural
dye anthocyanin-sensitized solar cells can potentially improve the
mechanical and environmental stability of DSSCs in addition to
enhancing their conversion efciency (Zhu et al., 2008). In another
experiment overall conversion efciencies of DSSCs fabricated with
natural sensitizers obtained from pomegranate juice for cells
operated with Pt 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 lm with natural dyes extracted
from C. indica L., Salvia splendens, cowberry and Solanum nigrum L.
as sensitizers. Dai and Rabani (2001, 2002) employed 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 available anthocyanins.
Sandquist and McHale (2011) explored the use of a blocking layer
and treatment by TiCl4 in order to optimize the performance of the
betanin-based dye-sensitized solar cells, and recorded the highest
energy conversion efciencies as high as 2.7% for a DSSC containing
a single unmodied natural dye sensitizer. In a combined experimental and theoretical study of natural betalain pigments Oprea
et al. (2012) identied betacyanins as the useful constituents of
red beetroot extract as natural sensitizers and emphasized on the
role of extract purication for better results. Kumara et al. (2006)
investigated synergistic sensitization by dye cocktail (shisonin
and chlorophyll) obtained from shiso leaves and successfully achieved broadening of spectral response of dye-sensitized solar devices. Synergistic effect of mixed pigments in the energy transfer of
the pigment sensitized mesoporous TiO2 solar cells was further
conrmed by experiments on DSSCs fabricated with mixed chlorophyll and xanthophylls pigments extracted from different plants
(Bao-Qi et al., 2008). Energy conversion efciencies and maximum
power output for solar cells sensitized by mixed pigments were
much higher than that achieved by the linear superposition of the
cells sensitized by individual pigments. Furukawa et al. (2009)
fabricated various DSSCs using natural dyes of red cabbage, curcumin, red perilla and their mixtures. They found that the conversion efciency 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.
321
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 lm is also a very important
factor in determining the performance of fabricated cells. They
reported that the energy conversion efciency of the TiO2 electrode
with successive adsorptions of gardenia yellow (GY) and gardenia
blue (GB) dyes was 0.59%, which is enhanced compared to single
dye adsorption (0.32% for GY and 0.16% for GB), however adsorption
of GY and GB dye mixture resulted in much lower energy conversion efciency (0.04%). The decrease in efciency of such cocktail
dyes due to unfavorable interactions between the two dyes.
Incorporation of a natural dye-sensitized solar cell fabrication
module in conventional science laboratory courses is an effective
approach, which provides an interdisciplinary, practical model for
students learning the basic principles of biological extraction,
chemistry, physics, environmental science, electron transfer and
photochemical technology (Smestad and Gratzel, 1998). Few researchers have taken into account the educational importance of
naturally sensitized solar cells and presented their experiments as
interesting multidisciplinary exercises for dissemination of
knowledge and to educate people on renewable energy resources
(Calogero and Marco, 2008; Raturi and Fepuleai, 2010; Smestad,
1998).
Despite the effort involved the in use of natural dyes as sensitizers, low conversion efciencies of these DSSCs would appear to
be unpromising from a commercial viewpoint. Although a number
of natural dyes have been tested for their performance in DSSCs
(Table 4), most of them yielded conversion efciencies of less than
1%. Betanin extracted from beet roots, h 2.71% (Sandquist and
McHale, 2011), Xanthomonascin-A extracted from Monascus purpureus, h 2.3% (Ito et al., 2010), and isobutrin from Butea monosperma, h 1.8% (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 efciencies over 2% (Calogero et al., 2009). Natural chlorophyll derivative chlorin-e6 exhibited energy conversion
efciencies over 4% (Ikegami et al., 2008). The efciency of natural
dye-sensitized solar cells is determined by a number of factors that
include selection of the appropriate natural dye, quantitatively
signicant stable electronic anchorage of the dye to the surface of
the metal oxide nanostructure, choice of photoanode, counter
electrodes, 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
option. The advantages of natural dyes as photosensitizers are
large absorption coefcients, high light-harvesting efciency, no
resource limitations, low cost, simple preparation techniques and
no harm to the environment. Although the efciencies obtained
with these 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 from
bioresources invoked participation of researchers around the globe
to engage in research to search for new sources of natural dye
systems that are stable, non-toxic, biocompatible and have desirable optoelectronic properties. Some serious efforts in natural dye
sensitizers may spring up a perspective of commercial feasibility for
inexpensive and environmentally friendly dye-sensitized solar
cells.
5. Natural dyes in food coloration
As a consequence of growing worldwide concern for food
quality and safety, a set of standards have been brought in by
TiO2 coated FTO
TiO2 coated FTO
TiO2 coated FTO
Pt coated FTO
Pt coated ITO
Pt coated ITO
Pt coated FTO
Counter electrode
LiI/I2/pyridine
LiI/I2
LiI/I2
LiI/I2/DMPImI/TBP
LiI/I2/TBP
Electrolyte
composition
Acetonitrile/propionitrile
3-Methoxypropionitrile
Acetonitrile/3-methyl2-oxazolidinone
3-methoxyprpionitrile
Acetonitrile
Propylene carbonate
Solvent system
Photoelectrode
TiO2 coated FTO
Pt coated FTO
0.84
0.74
0.60
0.96
0.85
0.14
1.02
0.90
2.69
0.97
0.51
0.85
1.19
3.56
3.52
4.80
3.84
3.4
0.63
0.74
1.61
0.53
0.51
1.36
1.03
2.95
2.42
2.00
0.81
0.39
0.56
1.06
0.86
0.37
9.5
9.4
2.7
2.1
6.1
1.0
3.9
5.45
4.40
4.04
2.46
1.31
1.15
0.58
0.518
0.609
0.554
0.572
0.616
0.337
0.498
0.483
0.686
0.595
0.498
0.559
0.607
0.55
0.432
0.534
0.340
0.350
0.537
0.592
0.585
0.689
0.542
0.522
0.484
0.357
0.44
0.22
0.53
0.51
1.55
0.39
0.422
0.442
0.425
0.350
0.375
0.300
0.49
0.59
0.45
0.392
0.406
0.400
0.408
0.403
0.402
Voc (V)
0.641
0.626
0.571
0.627
0.66
0.605
0.585
0.645
0.619
0.633
0.659
0.667
0.687
0.654
0.51
0.39
0.51
e
e
0.722
0.631
0.609
0.466
0.831
0.696
0.682
0.3
0.63
0.51
0.69
0.67
0.67
0.48
0.43
0.61
0.35
0.38
0.54
0.57
0.52
0.61
0.56
0.535
0.569
0.633
0.591
0.568
0.637
FF
1.8
0.27
0.26
0.21
0.36
0.32
0.03
0.33
0.27
1.17
0.38
0.17
0.33
0.47
1.01
0.59
1.31
0.50
0.40
0.24
0.28
0.57
0.17
0.23
0.50
0.34
0.402
0.67
0.19
0.60
0.27
1.17
e
e
e
1.7
1.26
0.50
0.36
e
e
e
1.14
1.02
1.02
0.59
0.30
0.29
Jsc (mA/cm2)
4.67
Reference
Zhang et al., 2008
Furukawa et al., 2009
Garcia et al., 2003a,b
Calogero et al., 2010
Patrocinio et al., 2009
Fernando and Senadeera, 2008
Oprea et al., 2012
Calogero and Marco, 2008
Zhou et al., 2011
Kumara et al., 2006
Agarkar et al., 2011
322
Dye
Molecular
structure
Table 4
Functional parameters of various natural dye-sensitized solar cells.
Red beet roots
TiO2 coated FTO
Acetonitrile/ethylene
carbonate
KI/I2
TBAI/I2
Pt coated FTO
KI/I2
Pt coated FTO
TiO2 coated FTO
Pt coated FTO
Acetonitrile
Ethylene glycol/
acetonitrile
Ethylene glycol/
acetonitrile
Acetonitrile
TiO2 coated FTO
Betailain
TiO2 coated FTO
DMPImI/
LiI/I2/TBP
DMPImI/LiI/
I2/GT/TBP
Pt coated FTO
Pt coated FTO
TiO2 coated FTO
TiO2 coated FTO
TiO2 coated FTO
e
e
e
e
e
e
e
e
e
e
e
e
e
Shisonin
Chlorophyll
Shisonin
chlorophyll
Isobutrin
Cyanine
Nasunin
e
e
e
e
e
e
e
Betanin
Betaxanthin
e
Shisonin
e
e
e
e
e
e
e
e
Anthocyanidins
Anthocyanidins
Anthocyanidins
Anthocyanin
e
e
e
e
e
Red cabbage:curcumin
Red perilla
Red cabbage
Chaste tree fruit
Morus alba
Euterpe oleraceaa
Beta vulgaris rubra
Opuntia engelmannii
Opuntia cus indica
Bougainvillea
Morus alba
Vaccinium myrtillus
Mirtus caulifora
Hibiscus surattensis
Sesbania grandiora
Hibiscus rosasinensis
Nerium oleander
Ixora macrothyrsa
Rhododendron
arboretum
Beet root
Citrus Sinensis
Solanum melongena L.
Begonia
Tangerine peel
Rhododendron
Fructus lycii
Marigold
Perilla
Herba artmisiae
scopariae
China Ioropetal
Yellow rose
Flower knotweed
Bauhinia tree
Petunia
Lithospermum
Violet
Chinese rose
Mangosteen pericarp
Rose
Lily
Coffee
Broadleaf holly leaf
Shisho leaves
Butea monosperma
Canna indica L.
Salvia splendens
Cowberry
Solanum nigrum
Bixa orellana
Black rice
Erythrina
Rosa xanthina
Kelp
Capsicum
Myrtus cauliora
Berberies buxifolia
Monascus purpereus
Gardinia fruit
Spinach extract
Ipomea leaf extract
Pomegranate leaf extract
Mulberry extract
Ixora coccinea
Mulberry
Beetroot
Delonix regia
TiO2 coated FTO
Pt coated FTO
DMPImI/
LiI/I2/TBP
0.54
0.61
0.54
0.59
0.31
0.37
0.13
0.01
0.017
e
e
e
e
e
e
e
2.3
0.56
0.16
0.131
0.278
0.597
0.548
0.722
0.26
0.13
0.29
TiO2 coated FTO
TiO2 coated
conductive
glass
Pt coated FTO
Pt coated ITO
Pt coated FTO
Pt coated
conductive
glass
Pt coated FTO
LiI/BMII/I2/TBP
KI/I2
LiI/I2
KI/I2
DMPImI/LiI/I2/TBP
Acetonitrile/3-methyl2-oxazolidinone
Acetonitrile/valeronitrile
Ethylene carbonate/
acetonitrile
e
Ethylene glycol/
acetonitrile
methoxypropionitrile
TiO2 coated FTO
TiO2 coated FTO

TiO2 coaoted FTO
Pt coated ITO
LiI/I2
ZnO coated FTO
TiO2 coated ITO

e
Pt coated ITO
Luo et al., 2009
0.82
0.558
0.556
0.51
0.59
0.64
0.37
0.34
0.52
0.55
0.52
0.62
0.63
0.54
0.36
0.66
0.46
0.60
0.51
0.563
0.52
0.53
0.49
Acetonitrile/
valeronitrile
0.7
0.4
0.54
0.57
0.53
0.32
0.34
0.551
0.484
0.492
0.441
0.412
0.59
0.47
0.57
0.43
0.58
0.55
0.54
0.56
0.555
0.53
ZnO coated ITO
Pt coated ITO
Acetonitrile
Acetonitrile
TiO2 coated ITO
LiI/I2
TiO2LiI/I2/PEO/TBP
LiI/I2
TiO2LiI/I2/PEO/TBP
Ce(NO3)3/Ce(NO3)3
KI/I2
Shanmugam et al., 2013
Hemalatha et al., 2012
Sandquist and McHale, 2011
Senthil et al., 2011
Thambidurai et al., 2011
Chang and Lo, 2010
Chang et al., 2010
Ito et al., 2010

Yamazaki et al., 2007
Polo and Iha, 2006
Hao et al., 2006
Gomez-Ortiz et al., 2010
1.01
1.1
0.38
0.087
0.15
1.142
0.776
0.637
0.433
0.225
9.0
6.2
6.1
2.84
0.45
0.467
0.914
2.05
1.89
2.8
Acetonitrile
Lai et al., 2008
Cyanidin3-scillabiose
Salvianin
Cyanidin3-galactoside
Anthocyanin
Bixin
Norbixin
Bixin
Norbixin
Anthocyanin
Carotenoid
Anthocyanin
Chlorophyll
Carotenoid
Anthcyanin
Anthocyanin
Xanthomonascin_A
Crocin
Crocetin
Chlorophyll
Chlorophyll
Chlorophyll
Anthocyanin
Chlorophyll
anthocyanin
e
e
e
Cyanidin3-O-glucoside
Anthocyanidin
0.33
0.41
0.28
0.317
0.245
0.505
0.444
0.454
Eugenia jambolana
0.29
0.30
0.3
0.39
0.48
0.48
0.46
0.364
Ethanol/water
0.21
0.23
0.2
0.30
0.30
0.35
0.30
0.249
Ag coated ITO
2.65
2.90
2.30
1.33
0.84
1.49
1.58
5
Zhu et al., 2008
Bogainvillea brasiliensis
0.691
1.18
1.49
1.46
Au Nanoparticle
loaded on
TiO2 coated FTO
0.331
0.289
0.273
0.42
TiO2 coated FTO
0.322
0.520
0.496
0.33
e
e
e
Anthocyanin
6.48
7.85
10.9
10.6
Garcinia suubelliptica
Ficus Reusa Linn.
Rhoeo spathacea
Black berry
LiI/I2
Tobin et al., 2011
Nanocarbon
coated FTO
Pt coated- FTO
2.71
2.22
e
TiO2 coated FTO
0.56
0.61
0.525
Betanin
0.36
0.44
0.403
Beet root
13.91
8.61
0.289
e
Anhydrous ethylene
glycol
Acetonitrile
3-Methoxyproprionitrile
e
TiO2 coated FTO
Park et al., 2013
Anthocyanins
0.32
Hibiscus owers
0.62
DMPImP/LiI/I2/TBP
0.54
Graphite
coated FTO
Pt coated FTO
Iodolyte AN 50 (Solaronix)
0.96
TiO2 coated FTO
Pt coated FTO
Gardenia yellow extract
TiO2 coated FTO
0.16
0.22
0.29
0.076
0.301
LiI/I2/TBP
0.69
0.6775
0.664
0.49
0.65
Pt coated FTO
0.44
0.5839
0.5433
0.644
0.495
TiO2 coated FTO
0.53
0.5597
0.8017
0.24
0.94
Geniposide, crocin,
crocetin
Crocin and crocetin
Xanthophyll
Anthocyanin
b-Carotene
Cyanidins
Gardenia blue extract

Kerria japonica
Rosa chinensis
Ivy gourd fruits
Red frangipani owers
e Not specied; FTO: uorine doped tin oxide; ITO: indium doped tin oxide; DMPImI: 1,2-dimethyl-3-propylimidazolium iodine; TBP: 4-tert-butyl pyridine; TBAI: tetrabutylammonium iodide; GT: guanidinium thiocyanate;
BMII: butylmethylimidazoliumiodide; PEO: polyethylene oxide.
323
324
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 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, extraction, purication, stabilization and standardization for a variety
of natural food colorants are available such as anthocyanins
(Wrolstad, 2004), betalains (Azeredo et al., 2009; Roy et al., 2004;
Stintzing and Carle, 2007), chlorophylls (Humphrey, 2004; Kong
et al., 2012), carotenoids (Mortensen, 2006), tannins (Vankar
et al., 2006), Monascus (Dufosse et al., 2005), quinones (Gonzalez
et al., 2002), biliproteins (Sekar and Chandramohan, 2008), safower (Cho et al., 2000), turmeric (Marcolino et al., 2011), etc. They
have different groups of chemical compounds which may be used
directly as colorants or in chemically modied form to produce
different hues ranging from green through yellow, orange, red, blue,
and violet, 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 choices
to give distinguished look and quality to a variety of food
preparations.
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 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 more attention to the development of natural food colors, as they are generally more internationally accepted (Burrows, 2009). Table 5 lists naturally derived
colorants approved by EU, USA and Japan for use in food coloring.
Downham and Collins (2000) portrayed a very illustrative picture
of future outlook of legislation, innovations in formulation and
processing 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
colors owing to a continued consumer pressure to go natural. The
production of many currently approved natural food colorants has
a number of disadvantages including 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 plants (Castellar et al., 2008; Longo and
Vasapollo, 2005; Lin et al., 2010) and insect (Gonzalez et al.,
2002; Borges et al., 2012) origin as well as other biological sources such as fungi (Duran et al., 2002; Mapari et al., 2005;
Velmurugan et al., 2010), bacteria (Zhang et al., 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 change, temperature and
prone to light, heat and oxygen disintegration (Delgado-Vargas
et al., 2000). Ascertaining the color stability of natural colorants
as prerequisite for their successful application a number of researchers focused on improving color stability of different classes
of natural food colorants (Castaeda-Ovando et al., 2009; Herbach
et al., 2006). Although, the wealth of information is now available
on new sources for food colorants, however, any new pigment
source would require rigorous assessment of established safety
tolerances and should meet the economic, legal and aesthetic requirements, for approval by food regulatory authorities (Downham
and Collins, 2000).
Pigments producing microbes such as fungi, bacteria and

microalgae are quite common in nature. Among the molecules
produced are carotenoids, melanins, avins, quinones and more
specically monascins, violacein, phycocyanin or indigo (Dufosse,
2006). A great upsurge 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 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 fungal food colorant has
tremendously increased the prospects of research to explore the
extraordinary chemical diversity and biodiversity of fungi for the
biotechnological production of pigments as natural food colorants.
Recent data indicate that with an appropriate selection 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 functionality and
expand the color palette of existing natural food colorants; the
fungal natural colorants could be produced in high yields by using
the available cultivation technology without potential genetic
manipulation since tougher legislation and skeptical attitude of
consumers make it rather difcult for the acceptance of genetically
modied food (Mapari et al., 2005, 2006, 2009, 2010). Microalgae
are also seen as a major natural source for a vast variety/array of
natural colors. Campo et al. (2007) presented a beautiful picture of
current state and future perspectives of carotenoid colorant production by microalgal cultivation. Carotenoid production has been
proved to be one of the most successful branches of biotechnology
of microalgae.
Innumerable associated benets and myriad therapeutic properties are linked with the use of natural colorants in food industry
(Chattopadhyay et al., 2008; Siva et al., 2011). For example, in
addition to coloring property, anthocyanin extracts may act as
quality control marker for foodstuffs; 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 (provitamin A agents) or as dietary supplements (Mortensen, 2006). Paprika is a source of vitamin C,
whereas riboavin 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 products, naturally derived food colorants may
improve the nutritional value of the target food. These prospective
nutraceutical properties may play increasingly important role in
making a choice between natural or synthetic food colors at a time,
where human diet is more and more based on processed foods
(Stintzing and Carle, 2007).
Appearance, consumer preferences and safety standards of
foods and food colors coupled with economics and application
technology will always play a key role in the success of new food
products. At one time, synthetic colors were the rst choice as food
colorants and natural colorants were relegated to a limited number
of traditional applications because of limited availability, difculty
in use, instability and high cost. The renewed interest in natural
food coloration is resulted due to stringent regulatory pressure, bad
325
Table 5
Approved naturally derived food colorants in European Union (EU), Food and Drug Administration (FDA) of USA and 7th edition of Japans Specications and Standards for Food
Additives (JSSFA).
EU Name
E-number
USA name
U.S. CFR number
JSSFA name
Colors obtained
Curcumin
E 100
Yellow
E101
73.600
73.615
73.450
Turmeric oleoresin and curcumin
Riboavin
Riboavin-50 -phosphate
Cochineal, carminic acid,
carmines
Chlorophylls and
chlorophyllins
Copper complexes of
chlorophylls and
chlorophyllins
Caramels
Vegetable carbon
Carotenes
Turmeric
Turmeric oleoresin
Riboavin
Yellow
E120
Cochineal extract, carmine
73.100
Cochineal extract and carminic acid
Pink to red
E140
Chlorophyll
Green to olive
E141
Sodium copper chlorophyllin
73.125
Bluish green
E150 (aed)
E153
E160a
Caramel
e
Carrot oil
73.85
Brown
Grey to black
Golden yellow to orange
Annatto, bixin, norbixin

Paprika extract, capsanthin,
capsorubin
Lycopene
E160b
E160c
b-Carotene
Annatto extract
Paprika, Paprika oleoresin
73.95
73.30
73.340
73.345
73.585
Caramel (aed)
e
Carotene from carrot
Carotene from palm oil
Carotene from Dunaliella
e
Paprika color and oleoresin
Orange
Reddish orange
Orange red
b-apo-8 -carotenal (C30)

Ethyl ester of b-apo-80 -
E160e
E160f
e
e
Reddish orange
Yellow/orange
carotenic acid (C30)

Lutein
Canthaxanthin
Beetroot red, betanin
Anthocyanins
E161b
E161g
E162
E163
73.75
73.40
73.169
73.170
Marigold color
e
Red beetroot
Grape skin color and extract
Blackcurrat color
73.140
Golden yellow
Orange pink
Pink to red
Depending on pH gives
a wide range of colors
varying from Pink/red to
mauve/blue
Brown
73.250
73.260
73.500
e
e
e
Monacus color
Carthamus red
Carthamus yellow
Varies
Varies
Orange Yellow
Red
Red
Yellow
e
e
e
e
e
e
e
E160d
Tomato lycopene extract,

tomato lycopene concentrate
b-Apo-80 -carotenal
e
e
Canthaxanthin
Dehydrated beets (beet powder)
Grape color extract
Grape skin extract (enocianina)
Toasted partially defatted cooked

cottonseed our
Fruit juice
Vegetable juice
Saffron
e
e
e
73.300
73.90
e Not included.
publicity for the synthetic food colors and need for globally
approved colorants (Frick, 2003). With biotechnological advances,
contemporary researchers are in a position to simplify the techniques for production of the existing colorants and nd new
colorant sources for their commercialization. By appropriate selection of new sources for known colorants, formulating new ways
for existing pigments and improvement of existing sources by
mutation or genetic engineering techniques better pigments production yield could be achieved. Although many advances in the
developments of natural food colors covering different aspects such
as extraction, purication, stability, identication of new sources,
formulation techniques 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 may have wider industrial applications.
6. Other applications of natural dyes
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 et al., 2004); to add color to cosmetics (Kapoor, 2005;
Kapoor et al., 2008); to dye hair (Boonsong et al., 2012;
Komboonchoo and Bechtold, 2009; Rao et al., 2008); to impart
color to some pharmaceutical preparations (Chigurupati et al.,
2002); and also in histological staining (Tousson, and AlBehbehani, 2011). Different prospects of natural colorants used
in/as cosmetics products are comprehensively reviewed by Dweck
(2002, 2009a,b). Natural pigments derived from different sources
with active functional components have shown high biological
activities, 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., 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 such as indigo
and anthraquinone-based colorants can be used in appliances
where moderate 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 photopolymerization of styrene is also reported (Mishra and Daswal,
2007). Siva et al. (2008) reported an easy, practical and reliable
procedure for using Bixa orellana L. natural dye as an 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 xation of the Microcapsules (MCs) containing
n-octadecane and n-eicosane on the back side of the fabrics using
the dot-screen printing method. They obtained relatively good
326
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 are also tested as safe TiO2-sensitizer for
photodegradation of organic contaminants in water purication
systems as a promising replacement for more costly and hazardous
heavy-metal based systems such as CdS particles and Rucompounds (Zyoud et al., 2011). Kuswandi et al. (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 curcumin immobilized on
bacterial cellulose membrane (biopolymers) can be used as a
package sticker sensor for the visual detection of shrimp spoilage
and could offer an extra analytical device both to the sh industries
and retailers who are interested in approaches and 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 isolated from R. emodi, revealing
the use of dye as an extrinsic probe to determine the thermal stability of proteins by exploiting the uorescence properties of
anthraquinone derivatives for their interactions with relevant
target proteins.
Researchers have lately explored the promise of some historical
pigments such as indigo and madder in designing novel organic
electronics devices successfully. Recent explorations on thin lms
of indigo and Tyrian purple have shown their good charge transport
properties for use in organic electronics as natural and sustainable
semiconductors. Indigo and Tyrian purple form highly ordered thin
lms 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, dielectric) they
demonstrate the possibility of creating fully biocompatible/biodegradable electronics for many low cost applications (G1owacki 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 batteries. The
lithium batteries assembled using purpurin and chemically lithiated purpurin (CPL) as working electrode showed good charge/
discharge characteristics with very good reversible lithium ion
storage properties. Future large scale application of sustainable
organic electronics based on biodegradable materials would have a
positive impact on the current problem of electronic waste.
These interesting ndings on newly discovered panoramas of
natural dye applications invoke great expectations for further
research on utilization of natural dyes in a wide variety of elds
with focus on the future industrial application.
7. Conclusion
Natural dyes, generally supposed to be cheap, non-toxic,
renewable and sustainable resource with minimal environmental
impact, have attracted the attention of the scientic community to
use them in a variety of traditional and newly discovered application disciplines. Although, past few years have witnessed substantial growth in our understanding of technological details
required for efcient utilization of colorants obtained from natural
sources, but still there are a number of technical challenges in each
area of natural dye application that must be overcome before these
technologies can be adopted on a practical large scale. Improving
methodologies of extraction and application and generating costeffective processes are 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 generated from these studies may
device the basis for the economic viability of natural dye production in commercial scale for sustainable utilization of bioresources.
Extensive R&D in 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 in different spheres of our life is a long term prospect.
Acknowledgement
Financial support provided by University Grant Commission,
Govt. of India; through BSR Research Fellowship in Science for
Meritorious Students (Mohammad Shahid) and Research Fellowship to Central University Ph.D. Students (Shahid-ul-Islam) is
thankfully acknowledged.
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Journal of Cleaner Production 53 (2013) 310e331

Contents lists available at SciVerse ScienceDirect

Journal of Cleaner Production

Recent advancements in natural dye applications: a review

* Corresponding author. Tel.: 91 9350114878.

human being towards a vast portfolio of possibilities (Dawson,

2. Technological advancements in textile coloration with

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

Fig. 1. Various applications of natural dyes.

Environmental concerns arising due to accelerated development in

improvement for natural colorant extraction (Bechtold et al., 2002;

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

Conventional metallic mordants

Park et al., 2005; Samanta and Agarwal, 2009;Vankar et al.,

Das et al., 2008; Moiz et al., 2010;Rekaby et al., 2009

Zheng et al., 2011

Newly discovered metallic mordants

shade ranges and better fastness properties (Kadolph and

is not new; yet the lack of well-documented research records on

Reason for use as

Mansour and Heffernan, 2011

Cu rich plant used as

Arroyo-Figueroa et al., 2011

Vankar et al., 2008d

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

galls. Phenolic hydroxyl groups of tannins enable them to form

all cases, and attributed it to enhanced shrink-resistance properties

Raja and Thilagavathi, 2011

Zhang and Cai, 2011

Montazer et al., 2009

Natural dyes used in the study

Grevillea robusta, Spathodea campnulata,

Terminalia Arjuna, Punica granatum, Rheum

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

processing. Ultrasound can improve effectiveness of a wide variety

# Energy savings by dyeing at lower temperatures and reduced

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

modication of cotton fabric with reactive cyclodextrin (R-CD) at

currently most of the studies are based on laboratory results or

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

coloring substances in olive oil producing countries which are

is expected to contribute to sustainable development in the near

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

e.g. Indigo, Madder,

EXTRACTION AND STANDERDIZATION

WASTE WATER CONTAINING

pathogenic gram positive and gram negative bacteria (Gupta et al.,

grandis, Morinda citrifolia (Prusty et al., 2010), Albizia lebbek and

M. Shahid et al. / Journal of Cleaner Production 53 (2013) 310e331

Turmeric (Curcuma longa)

Indian Rhubarb (Rheum emodi)

R1 =OCH3, R2 = OCH3 Curcumin

Weld (Reseda luteola)

R1=H, R2=CH3 Chrysophanol; R1=H, R2=CH2OH Aloe-emodin

Eucalyptus (Eucalyptus globulus)

Cutch (Acacia catechu)

Flos sophorae (Sophora japonica)

Onion (Alium cepa)

Gallnut (Quercus infectoria) &

Indigo (Indigofera tinctoria)

Cochineal (Dacylopius coccus)

Jackfruit (Artocarpus heterophyllus)

Teak (Tectona grandis)