High-Energy Radiation Induced Sustainable Coloration and

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High-Energy Radiation Induced Sustainable Coloration and Functional Finishing of Textile Materials Shahid-ul Islam, and FAQEER MOHAMMAD Ind. Eng. Chem. Res., Just Accepted Manuscript • DOI: 10.1021/acs.iecr.5b00524 • Publication Date (Web): 31 Mar 2015 Downloaded from http://pubs.acs.org on April 4, 2015

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Industrial & Engineering Chemistry Research

High-Energy Radiation Induced Sustainable Coloration and Functional Finishing of Textile Materials Shahid-ul Islam, and Faqeer Mohammad* * Corresponding author Department of Chemistry, Jamia Millia Islamia (A Central University), New Delhi-110025, India Phone: +91-9350114878. E-mail: [email protected]

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Abstract Over the past few years, there has been enormous attention on the use of different innovative surface modification methods for the production of textile surfaces with novel properties. In view of the ecological and economic restrictions imposed on the textile industry, the use of high energy irradiations methods has become more accepted as methods for modification of textile materials. Enhanced wettability, dyeability, printability, color fastness, hydrophilicity, and effective antimicrobial activity etc are among some new remarkable properties obtained on different textile materials. They offer a new alternative to conventional wet processing technologies and have the advantages of low energy use, easy to handle and high treatment speed. They possess the potential to activate textiles surfaces and hence enhance functional group accessibility without affecting other bulk properties. The present review summarizes the state of the art of different irradiation based technologies such as gamma, ultrasound, plasma and ultraviolet used for sustainable coloration and functional finishing of different textile materials. Finally, the advantages and future studies regarding the use irradiation technologies in functional modification of textiles are also outlined.

Key words: Radiations; Gamma, UV protection; Coloration; Antimicrobial activity


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1. Introduction The advancement of technology and increasing global competition in textile market has lead scientists and technologists to look for or develop novel finishes of high add value on different textile materials. The rapid growth in textiles have opened new windows for the scientists to advent and explore new research fields which include geo-textiles, flame retardant textiles , insect repellent textiles, aroma textiles, medical-textiles, smart textiles and nano-textiles etc.1-4 Globally, scientists are now devoting special attention to these fascinating fields of textile research and extensive research works and many patents have been reported in literature dealing with a wide range of compounds applied to different areas of textile finishing.5-10 It is well known that natural fibres particularly cotton; wool, silk, viscose and linen and synthetic fibres are most widely used in textile industry today for a wide range of applications.11 Cotton textiles with a superhydrophobic finish are particularly an attractive choice in many water proof and self cleaning apparel.12-14 Furthermore, demand from consumers for textiles with self cleaning, antimicrobial,15-17 UV-protective,18-20 waterproof,21 anti-felting, anti-shrinking, mothproofing,22, 23 flame retardant, and stain resistant properties is growing stronger. This has substantially increased scientific activity in production or for application of innovative chemical agents on different textile surfaces. Use of different agents such as quaternary ammonium compounds,24,

25

N-halamine siloxanes,26,27

heterocyclic compounds with anionic groups, polyhexamethylene biguanide, triclosan, metals, synthetic dyes,28, 29 natural products such as biopolymers,30-32 and natural colorants11, 33-35

have gained significant academic and industrial interest in producing antimicrobial

textiles for various medical and hygienic applications. Lately, scientists have explored the potential of nanotechnology to alter physico-mechanical, optical, electrical and biological properties of various textile materials.36 Several researchers have recently discovered new 3 ACS Paragon Plus Environment


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advantageous functions on textiles finished by using silver, titanium dioxide, and zinc oxide nanoparticles.37-40 They have been sought to improve existing properties and produce textile materials with diverse practical performance which undoubtedly are greatly appreciated by demanding consumer market. In spite of numerous potential applications of multifunctional textiles in various industries notably in textile, pharmaceutical, medical, agricultural, and food, however surveys show little research work has been done so far on the effectiveness and durability of obtained effects preventing their exploitation on an industrial scale.37, 41 Additionally, the inefficient binding of colorants, metals and other finishing agents onto textile materials can cause their release in the waste water of textile industries which can have lethal effects on all forms of life.42-44 Currently a number of methods including ion exchange, membrane filtration, advanced oxidation, biological degradation, photocatalytic degradation, electro-coagulation and adsorption are at operation for removing or minimizing these wastes.44-46 However, the treatment process of these waste waters using conventional methods has proved to be markedly ineffective, very difficult, and highly expensive. Table 1 summarizes molecular formulas and chemical structures of some common synthetic azo dyes present in textile waste waters. The insufficient binding of finishing agents and textile materials has now motivated research activities towards developing more-efficient and innovative methods for surface modification of textile materials. Recent developments in textile industry are mainly focused on modification of textile surfaces using various pre and post-treatment agents for improvement in color, and functional characteristics. Various chemical and biological methods, such as use of water insoluble polymers,47 imidazolidinone,48 chlorination,49 cross linking agents,50 enzymes,51 or ammonia treatments52 have been used effectively to improve or impart permanent functional properties


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on the surface of textile materials. However, such methods either rely on toxic chemicals or dangerous processes thus pose considerable energy and environmental challenges. Alternatively, radiation technology involving low energy use, no chemicals, easy to handle, and high treatment speed can modify the surface of textiles improving adhesion, wettability, dyeability, printability, fastness properties, resistance to easy wrinkling, washing and susceptibility to microbial attacks etc (Figure 1). In view of these facts, current review is intended to concentrate on some of the latest approaches dealing with the use of radiationinduced coloration and functional modification of textile materials for producing durable high added value textile materials which may be able to fulfill the consumer’s desire for a healthier and a more productive lifestyle and may find potential commercialization in the textile industry. 2. Irradiations Technologies Textiles wet production processes such as sizing, scouring, bleaching, mercerizing, dyeing, printing, and finishing are characterized by a huge consumption of water, energy, and chemicals.

53-55

At present, however the development of efficient clean radiation based

technologies as alternatives to conventional wet processes to promote sustainable production of textiles has become a major focus of textile researchers. Irradiation technologies offer several advantages in terms of energy saving (low-temperature process), low environmental impact, easy to use, economical and high treatment speed and therefore are gaining more popularity for use in textiles industry (Figure 2).56-58 Surface modification of fibre surfaces by using irradiation methods particularly gamma, ultrasonic radiations, plasma and ultraviolet (UV) etc are a gaining a wide spread emerging interest for use in textile coloration and finishing as novel treatments without affecting other bulk properties. Several advantages and disadvantages of all these irradiation methods are listed in Table 2.



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2.1. Gamma irradiation technology Gamma rays are high energy electromagnetic radiations having energies above 100 keV and wavelengths less than 10 picometers. Surface modification of fibre surfaces using gamma irradiation technique is nowadays considered to be one of the promising methods.59 They offer several advantages in textile dyeing and finishing such as improved dye uptakes, producing deeper shades, more rapid fixation of dyes and increased wettability of hydrophobic fibres. Gamma irradiation adds value in coloration of textiles at low temperature without affecting the morphology of dyes as well as other properties of fabrics.60 Bhatti and colleagues61 reported that the application of gamma irradiation on cellulose fabric had been an effective way in tuning the cellulose surface for enhanced dye uptakes and for adhesion of vat green dyes. Also, the dyeing behaviour of cotton irradiated with gamma radiations using reactive black-5 dye powder has been investigated by Bhatti et al.62 In their work, the bleached and plain weaved cotton was irradiated to different absorbed doses of 100, 200, 300, 400, 500 and 600 Gy using Co-60 gamma irradiator and it was found that 500 Gy is most effective dose for enhancing color strength and fastness properties. In recent years the development of gamma irradiation treatments as alternative to chemical methods in natural dyeing particularly for extraction and application of dyes has opened new windows for researchers working in the field of textiles. Up to date several studies have been carried out dealing with the use of gamma irradiations to improve dye extraction and fastness properties of naturally dyed textile substrates. Naz et al63 noticed that the extract of irradiated eucalyptus bark improved the fastness properties of gamma treated cotton and that the pre and post treatment using mordants such as chrome alum, potassium dichromate, copper sulphate, ferrous sulphate, and stannous chloride increased the uptake of extract by cotton.

eucalyptus bark

Rehman and co-workers64 studied the dyeing behaviour of gamma

irradiated cotton fabric using lawsone dye extracted from henna leaves (Lawsonia inermis).


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They irradiated cotton and dye powder to different absorbed doses of 2, 4, 6, 8 and 10 kGy using Cs-137 gamma irradiator and found that gamma ray treatment has significantly improved the color strength as well as enhanced the rating of fastness properties of henna dyed cotton. In a subsequent publication Rehman et al65 reported the use of gamma irradiation for studying the dyeing properties of cotton using natural flavonoid dye extracted from irradiated onion shells (Allium cepa) powder. They found optimal absorbed dose for extraction of natural quercetin from onion shells to be 4 kGy. Optimum dyeing conditions to get maximum color strength and acceptable color fastness properties were found at 60 °C, material to liquor ratio of 1:30 using 10% alum as pre-mordant and 6% alum as post-mordant. Batool et al66 reported the influence of gamma radiations on dyeing behaviour of cotton fabrics using chicken gizzard leaf extract. The authors used Cs-137 as a source for gamma radiations and observed that a 10 kGy absorbed dose was most effective for dye extraction and in improving the dye uptake ability of fabric as well as color fastness properties. Bhatti and co-workers67 carried out the dyeing of cotton to improve the color strength and fastness properties by irradiating the turmeric powder and cotton fabric using Co-60 gamma irradiator. It was shown that gamma irradiation had drastic effect on light, rub and wash-fastness properties of turmeric dyed cotton. Ajmal et al68 studied the application of gamma irradiations to improve the extraction of colorant from pomegranate peel extract and to enhance color strength of dyed silk fabrics. Pomegranate (Punica granatum L.) peels are abundantly available as wastes and have great potential to be used as textile dyes. The irradiated silk dyed with pomegranate peel extract showed good color fastness properties. The pomegranate peel dyed silk fabric that had been irradiated and pre and post treated with aluminium, chrome, copper sulphate and tannic acid mordants showed notably better color strength and fastness properties. More recently, Khan et al69 investigated the dyeing of cotton with red calico (Alternanthera bittzickiana) leaves as natural colorants using different doses



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of gamma radiations (5, 10, 15, 20 and 25 kGy) in order to improve the depth of shades and fastness properties. It was interesting to observe that gamma radiations particularly, 15 kGy dose delivered best results and optimum dyeing conditions which produced good color strength were found to be 60 oC for 50 min, dye bath of pH 7.0 and salt concentration of 6 g/L. The chemical structures of coloring compounds isolated from some potential natural dye yielding plants by using gamma irradiation are shown in Figure 3. Table 3 also summarizes the optimum doses and dyeing conditions for high color strength and better fastness properties. 2.2. Ultrasound-assisted Coloration and Finishing Ultrasound technology is among irradiation technologies whose applications in medical sector, leather processing and environmental protection have soared in recent years.70-72 Literatures have shown that ultrasound in textile wet processing have numerous beneficial effects.56,73,74They can improve effectiveness of a wide variety of chemical and physical processes mainly by generating cavitation, the phenomenon of expansion and collapse of micro bubbles in the liquid medium.57,75 Several previous investigations have shown that ultrasonic technology enhances mass transfer during some textile processing steps such as desizing, 76,77 scouring,73,78,79 bleaching, 80, 81 mercerizing and dyeing of natural fabrics.82 The presence of contaminants in raw wool and cotton such as

natural grease/wax, vegetable

matters, waxes, pectins, pigments and reducing sugars has been a cause of major concern among scientific community. Conventional methods currently available for wool and cotton scouring consume a lot of chemicals, water and energy and are proving to be ineffective and highly expensive. To overcome this problem, Bahtiyari and Duran78 reported that application of ultrasound causes significant reduction in dirt removal from raw wool. Likewise, Eren and Erismis83 investigated the effect of ultrasound to obtain more efficient removal of impurities from biscouring of cotton by alkaline pectinase. They found that in the presence of ultrasound


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mainly from ultrasound homogeniser resulted in more efficient scouring of cotton and did not produce any significant change in the fibre structure. Ultrasound assisted dyeing was done as an alternative effective method to conventional dyeing of nylon-6 with Reactive Red 55 dye.84 Akalin et al82 studied the effect of ultrasonic energy on the wash fastness of three reactive dyes namely Reactive Red 58, Reactive Red 195, and Reactive Red 242 having three different reactive groups in their chemical structures. Sun et al85 reported that the dyeing of natural cotton in presence of ultrasound results in increased dye uptake and color strength of dyed cotton fabrics. McNeil and McCall86 reported the use of ultrasound in wool dyeing and finishing. It was observed that ultrasound did not cause any surface damage and had the potential to reduce the chemical and energy requirements of wool dyeing with reactive and acid milling dyes. Ferrero and Periolatto,75likewise, reported similar results for wool dyeing with acid levelling dyes using power ultrasound. Parvinzadeh et al87 investigated the effects of ultrasonic energy on the processing of cotton with a cationic softener and found better results than conventional heating. Besides it is worth to noting that at present natural dyes have shown huge potential in both research fields and textile industries due to their environmental friendly attributes. Ultrasound is reported to be beneficial in natural dyeing by providing easy efficient route for extraction of natural colorants, enhancing mordanting, and dyeing process.88 Sivakumar et al.89 studied the effect of power ultrasound in the extraction of natural dyes from green wattle bark, marigold flowers, pomegranate rinds, 4’o clock plant flowers and cocks comb flowers and found that there is about 12–100% improvement in percentage yield of extract as compared to magnetic stirring at 45 ◦C. Rahman and coworkers90 used ultrasonic cleaner for the extraction of natural dyes from heartwood and bark of Xylocarpus moluccensis plant. They reported that the ultrasound technology is more effective in extracting colorants compared to traditional boiling method. The extraction of natural colorants from pomegranate rind using ultrasound assisted extraction has also been



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reported by Tiwari et al.91 Several research papers about the application of natural dyes using sonication methods have been published by a group led by Vankar. Vankar et al 92 reported a study for the dyeing properties of Eclipta alba plant extract on cotton using ultrasound dyeing bath. More than 7-9% higher efficiency was found than conventional dyeings. Vankar and co-workers93 also studied the dyeing potential of Terminalia arjuna, Punica granatum, and Rheum emodi natural dyes on cotton and silk pretreated with enzymes namely proteaseamylase, diasterase and lipase using ultrasound and conventional heating. They found that the best results were obtained for cotton and silk fabrics pretreated with enzymes and dyed using sonication. Vankar and Shankar94 noticed that the use of ultrasound exhibits 39 and 52% increase in dye exhaustion of cotton dyed with extracts of Acacia catechu and Tectona grandis respectively, and that the pre-treatment with enzymes improved the dye adherence, wash fastness and light fastness on the cotton fabrics. Dyeing properties of Rubia cordifolia on cotton using sonicator has also been investigated. The cotton fabrics pretreated with biomordant Eurya acuminata DC var euprista showed very good fastness properties.95 In addition to enzymes and biomordant pre-treatments Vankar et al96 also studied the effect of metal ions on dyeing properties of cotton, wool and silk fabrics with colorants extracted from Symplocos spicata using ultrasonic energy. They found that the use of metal mordants plus sonicator bath results in high dye uptake and better fastness properties.

Mansour and

Heffernan,88observed the good colorimetric properties, light fastness and improved dye uptake of silk pretreated with alum and catechu mordants and after wards dyed with Sticta coronate lichen using ultrasound technology. In addition to silk environmental and energy efficient dyeing of wool fabric using alum mordant followed by dyeing with sticta coronate lichen under ultrasonic energy and glucose/hydrogen peroxide based redox system has revealed better results.97 In the year 2008, Vankar et al98 studied the sonicator dyeing of modified cotton, wool, and silk with Mahonia napaulensis DC. They reported that the


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sonication results in enhancement of dye uptake by 18%, 25% and 23% with alum mordant for cotton, silk and wool, respectively. Likewise Guesmi and co-workers99 reported the use of ultrasound for improving dyeability and for enhancement in fastness properties of modified acrylic fabrics dyed with indicaxanthin natural dye isolated from fruits of Opuntia ficusindica. Ultrasound technology has also been used to study the dyeing and fastness properties of modified cotton fabric using isosalipurposide dye; a purified chalcone isolated from Acacia cyanophylla yellow flower.100 Figure 4 shows some chemical structures of coloring compounds obtained from plant dyes by using power ultrasound. In a series of experiments Kamel and workers101, 102 have reported improvement in dyeing efficiencies and fastness properties of wool and cationized cotton with two insect based natural dyes namely lac and cochineal respectively. The chemical structures of main coloring compounds from both these insect dyes are shown in Figure 5. Moreover, the recent amalgamation of ultrasound irradiation and nanotechnology has further boosted the role of sonochemistry to develop multifunctional textiles on a large scale. Sonochemical irradiation has proven to be a simple, green, and cost effective technique for the synthesis of nanomaterials as well as for deposition of diverse nanoparticles onto various textile materials. Emerging evidence suggests that the sonochemical deposition of nanoparticles results in production of textile materials with durable multifunctional effects. Akhavan and Montazer103 reported sonochemical formation and deposition of titanium dioxide nanoparticles on cotton fabrics for achieving durable self-cleaning and UV-protection properties. Harifi and Montazer104 more recently published a review paper focused on the sonosynthesis of nanomaterials on textiles substrates and hence, this paper will not discuss in detail about the application of various nanoparticles in this realm. Some of the outstanding research works conducted on the in situ generation of nanomaterials such as silver, nano titanium dioxide, zinc oxide, and copper oxide and their subsequent coating on textile



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materials using ultrasound irradiation has been mainly contributed by different research groups led by Gedanken105-111 and Montazer.104, 112, 113 Perelshtein and colleagues114 applied ZnO nanocrystals with average size 30nm generated in situ through a sonochemical reaction on cotton bandage to study the antimicrobial activity of deposited particles against E. coli and S. aureus cultures. Zinc oxide nanoparticles synthesis was explained through the formation of ammonium complex as depicted in (1) and (2). They found that nanoparticles of ZnO deposited on cotton bandage yields strong bactericidal activity.

[Zn (NH3)4]2+ (aq) + 4H2O

Zn2+(aq) + 4NH3 . H2O (aq)

(1)

ZnO (s) + 4NH3 . H2O (2)

[Zn (NH3)4]2+ (aq) + 2OH-(aq) + 3H2O

The same group of authors also reported that ultrasound irradiation results in homogeneous distribution of the MgO and Al2O3 nanoparticles without any aggregation on cotton bandages and discovered that surface of cotton bandages loaded with MgO and Al2O3 nanoparticles shows bactericidal activity against E. coli and S. aureus cultures.115 The mechanical properties showed that the sonochemical treatment did not cause any significant damage to the yarn (Figure 6). Likewise, this group also introduced cellulose pretreatment in order to increase the adhesion of small sized ZnO nanoparticles synthesised by sonochemical method on cotton fabrics. It was observed that the enzyme pretreated cotton and deposited with ZnO nanoparticles had strong antibacterial activity which was maintained even after being exposed to 10 laundering cycles at 92 oC.110 2.3. Plasma-Induced Functional Finishing of Textile Materials Plasma is an innovative ecofriendly technology for the development of durable multifunctional effects on a wide range of textile substrates.116, 117 Over the past few years, 12 ACS Paragon Plus Environment

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plasma treatments are playing extraordinary role in coloration and functional finishing of textiles as they do not require water and produce any residual effluents.118,

119

Plasma

consists of excited and energetic species such as ions, radicals, electrons and metastables which are produced by the interaction of electromagnetic field with gas under appropriate pressure. Depending upon the appropriate choice of gas and control of operating conditions plasma technology can be used effectively in imparting enhanced wettability, dyeability, printability, color fastness, adhesion properties, hydrophilicity, and effective antimicrobial properties etc to different textile substrates.120-127 Numerous approaches have been attempted to critically study the plasma based grafting for improvement of antistatic properties for a wide variety of textile materials. Chongqi et al128 and Bai and Liu129 are among the researchers who have studied that grafting of poly(acrylic acid) and diallyldimethylammonium chloride onto polyacronitrile

and polyester fibres

respectively using plama discharge results in improved antistatic property. In other investigation carried out by Samanta et al,130plasma treatment was used for imparting effective antistatic finish on nylon and polyester fabrics. More recently, Hassan131 in a research experiment modified wool fabrics by corona plasma prior to bonding with a fibre reactive quaternary ammonium compound, 2, 3-epoxypropyltrimethylammonium chloride (EPTAC) to enhance antistatic and mechanical properties of wool. Samanta and colleagues132 investigated the influence of a stable milky white glow plasma (generated at atmospheric pressure in the mixture of gaseous reactive monomer-1,3-butadiene and He) in the reaction of 1,3-butadiene with cellulosic on durable hydrophobic functionality of cellulose fabric (Figure 7). Panda et al,133 likewise, described the effect of He/dodecyl acrylate plasma on hydrophobic functionalization of cellulose substrate. Ramamoorthy and co-workers134 studied the graft polymerisation of non-C8 fluorocarbons to previously plasma treated cotton fabrics for the preparation of water, alcohol, and oil repellent textiles. Samanta et al135 also employed



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cold plasma with bulk temperature being at room temperature for water and oil absorbency functionalization of nylon and polyester fabrics. SEM micrographs and AFM analysis revealed the formation of nano-sized channels on textiles surface after plasma treatment.

Textile materials especially based on cotton find extensive use in domestic applications. However they are prone to catch fires and this has compelled scientists to find ways to render textile materials less flammable. Many investigations are concerned dealing with the use of plasma-induced graft-polymerization of acrylate monomers bearing phosphate and phosphonate groups on the surface of PAN (polyacrylonitrile) textiles in order to reduce flammability of PAN textiles.136

Tsafack and Grutzmacher,137 likewise, also studied the

effects of simultaneous grafting and polymerization of four acrylate monomers namely diethyl(acryloyloxyethyl)phosphate (DEAEP), diethyl-2- (methacryloyloxyethyl)phosphate (DEMEP),

diethyl(acryloyloxymethyl)phosphonate

(DEAMP)

and

dimethyl(acryloyloxymethyl)phosphonate and two newly synthesised phosphoramidate monomers, diethyl(acryloyloxyethyl)phosphoramidate (DEAEPN) and acryloyloxy-1,3bis(diethylphosphoramidate) propan (BisDEAEPN) on cotton fabrics using argon plasma technology.

Furthermore, these authors observed that the use of acrylate and

phosphoramidate monomers results in good wash durability of the flame retardant finish on cotton. In another investigation, the same authors used argon plasma to graft flame retardant monomers (acrylate phosphate and phosphonates derivatives) and CF4 plasma treatment or Ar plasma to graft 1,1,2,2, tetrahydroperfluorodecylacrylate with a view to develop flame retardant and waterproof finish on cotton.21 Lam et al138 studied the application of an organic phosphorus compound (Pyrovatex CP New, FR) to previously plasma modified cotton for the preparation of flame retardant cotton textiles. They used melamine resin as a cross-linking agent, phosphoric acid as catalyst and zinc oxide as co-catalyst and found that treated cotton effectively displays durable flame retardant properties. 14 ACS Paragon Plus Environment

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Plasma technology has been also used as a dry and clean process for blend fabrics to achieve multifunctional properties. In a research investigation, Palaskar et al139 has suggested the use of plasma induced hexamethyldisiloxane polymer on polyester/cotton blended fabric in order to impart it water repellent property. Davis and colleagues140 activated the cotton/PET blend fabric using pressure plasma prior to deposition of vaporized fluorocarbon based monomers, 1,1,2,2-tetrahydroperfluorodecyl acrylate (THPFDA) and 1,1,2,2-tetrahydroperfluorododecyl acrylate and then graft polymerised the monomers with a second plasma exposure to study the water repellent and antimicrobial activity. They believe that the plasma induced-graft polymerization

and

use

of

antimicrobial

agents,

in

the

treatment

such

as

diallyldimethylammonium chloride (DADMAC), and a quaternary ammonium salt could lead to enhanced activity against gram positive and gram negative bacteria.

Some rigorous pieces of research has been conducted on modification of textile materials to introduce hydroxyl, carbonyl and carboxyl groups onto textile surfaces possibly due to oxidation and etching reactions and to

improve surface roughness for better adhesion

property.141-144 For example, Vesel et al145 found that applying RF oxygen, or nitrogen plasma for 5s on samples of pure viscose textiles increased the concentration of existing as well as formation of oxygen functional groups, while as hydrogen plasma resulted in reduction of hydroxyl groups on cellulose. Plasma treatment has been used to enhance the adhesion between polypropylene materials and polyvinyl acetate.146 Leroux and colleagues147 have observed that the use of atmospheric air plasma treatment based on dielectric barrier discharge (DBD) technology results in formation of polar groups on polyester surfaces which enhanced it adhesion with silicone resin containing adhesive primer. DBD technology has also been used by Oliveira and colleagues148 to study its effect on adhesion of phase-change material (PCM) microcapsules on wool fabric. XPS analysis of the DBD modified wool showed higher concentration of oxygen and introduction of more polar groups on the wool 15 ACS Paragon Plus Environment


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surface (Figure 8). The treated samples showed improved hydrophilicity and that the plasma technology enhanced wash durability of microcapsules on wool. In another study, Bozaci et al149 have studied the effects of argon and air atmospheric pressure plasma on adhesion of flax fibres with high density polyethylene (HDPE) and unsaturated polyester and found that air plasma result in a better adhesion of flax fibre and unsaturated polyester. It has been reported that atmospheric pressure plasma jet (APPJ) treatment in presence of ethanol pretreatment on the surface of ramie fibres can improve their adhesion to polypropylene.150 Moreover, Yaman and colleagues151 reported the grafting of 6-aminohexanoic acid (6-AHA), acrylic acid (AA), ethylendiamine (EDA), acryl amide (AAMID) and hexamethyldisiloxane (HMDS) compounds onto polypropylene fabric using argon plasma as a method for improved dyeability of polypropylene with acid and basic dyes. Jinka et al152 studied the use of atmospheric pressure plasma treatment (APT) for processing of cotton non woven fabrics and found that APT could be a viable alternative to caustic soda for dewaxing cotton. FT-IR spectrum revealed diminishing of peak intensities particularly in the region between 3000 and 2800 cm−1 after plasma treatment which confirmed that plasma had a strong influence on dewaxing of non woven cotton (Figure 9). Despite several advantages of wool, it has scales on surface which hinder in dyeing and introduce problems such as felting in wool industry.153 To overcome these problems, although many chemical treatments are available in market today however most of the chemical methods generate

effluents containing substantial amount of chloro-organic

compounds, by-products, and other auxiliaries which pose environmental concerns.154 It has been reported that plasma technology can be successfully used to enhance the hydrophilicity and surface electrostatic properties of wool fabrics and can improve its dyeing rate.155-158 Plasma irradiation has the potential to be used as a green technology to develop hydrophobic coating on cellulosic materials with various beneficial properties for textiles such as water


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proof and self cleaning activity.159, 160 Kamlangkla et al161 used radio-frequency inductively coupled SF6 plasma on cotton surface to enhance its mechanical strength and hydrophobicity. Furthermore, in a study, the possibility of increasing surface hydrophilicity and energy of grey cotton using low pressure discharge plasma has been proposed. FT-IR spectrum peaks revealed that the formation of polar groups on cotton surface had been mainly responsible for the enhancement of hydrophilicity.162 In addition, Cireli et al163 studied the hydrophilicity, wrinkle recovery and breaking strength properties of polyester and polyamide fabrics in presence of acrylic acid as precursor after being activated by low frequency plasma and discovered that the treatment results in enhanced surface properties. Several investigations have already been undertaken and are currently underway on the use of plasma technology in natural textile dyeing and finishing. Shahidi and co-workers164 have reported the use of thymol in the development of antibacterial cotton fabric which was modified by plasma treatment. The plasma pretreated cotton portrayed encouraging antibacterial results with a high wash durability. Kerkeni and colleagues165 studied the curcumin dye uptake of polyester fabric previously activated by plasma and UV excimer lamp treatment. Barani and Maleki166 used response surface methodology (RSM) to optimize dyeing conditions of wool with madder natural dye in the presence of chemical and physical modified natural soybean lecithin. They found that the application of plasma and acetylated lecithin improved the color strength significantly; however unsatisfactory results were obtained for hydroxylated-acetylated lecithin indicated from the lower K/S values of madder dyed wool. Barani and Rahimpour 167 reported the dyeing properties of Prangos ferulacea on wool substrate using response surface methodology (RSM) for optimization of various variables. The effect of plasma pretreatment and other variables such as dye concentration, mordant concentration, dyeing temperature, and time on color strength and fastness properties was also investigated. The dyed wool showed improved properties in presence of



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plasma and mordants. Haji and colleagues168 successfully applied berberine extracted from Berberis vulgaris as an effective antibacterial natural colorant on nylon 6 pretreated with low temperature plasma and mordanted with copper sulphate. It was observed that the resultant nylon 6 fabric shows high color strength and displays acceptable antibacterial activity against both gram-negative and gram-positive bacteria. Ismal and co-workers

169

studied the

feasibility of replacing metallic mordants with plasma treatment in natural dyeing of wool using almond shell as natural novel colorants. Nithya and co-workers170 introduced synergistic effect of low temperature plasma and enzyme treatments in order to increase antimicrobial properties of cotton fabric. In their research work, DC air plasma (P), cellulase enzyme (E), enzyme preceded by plasma (PE) and plasma preceded by enzyme were used before being treated with neem leaf extract. The resultant cotton fabric showed high antimicrobial activity against Staphylococcus aureus and Escherichia coli organisms. Kerkeni et al171 reported incorporation of nisin onto woven polyester fabrics preactivated by plasma to assess antibacterial effects of treated samples S. aureus. Ibrahim et al172 have described UV protective and antibacterial properties of linen fabrics obtained by a new method, based on modification of linen surface and creation of new functional sites using oxygen or nitrogen plasma and after treatment with ionic dyes, certain metal salts, nano-scale metal or metal oxides, and quaternary ammonium salt or nominated antibiotics. To date, a lot of research has been conducted on chitosan which is an effective antimicrobial finishing agent for textile modifications; however its weak binding capacity with textile surfaces constitutes the main problem in its applications.31 To overcome this problem a variety of methods have been tested for strong binding of chitosan to textiles. Among the new methods being developed, plasma technology is one of the most promising methods that have


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shown encouraging results on the application of chitosan in textile dyeing and finishing. Zemljic et al173 reported the influence of chitosan introduction onto cellulosic fabrics preactivated with oxygen plasma on antimicrobial activity. They believe that the plasma treatment enhanced hydrophilicity by the introduction of new functional groups due to oxidation reactions. It was concluded that the high adsorption of chitosan onto plasma activated fabric results in better inhibition against Streptococcus agalactiae and fungal pathogens such as Candida albicans and C. glabrata. Zhou and Kan174 studied the effect nitrogen plasma followed by chlorination with sodium hypochlorite on the antibacterial activity of cotton. The authors discovered that the nitrogen plasma introduced nitrogen containing groups into cotton structure, enhanced chitosan deposition and in presence of chorine inhibited the bacterial growth effectively. Tseng and colleagues175 grafted chitosan into the structures of nylon textiles prior to activation by open air plasma treatment. They claimed that air plasma activation of nylon at a speed of (26 m/min) for a few time enhanced grafting of chitosan which consequently showed good antibacterial activity. In textile dyeing and finishing, incorporation of nanotechnology is a new concept which has been introduced in recent years. Due to their extremely large surface area and high surface energy, nanoparticles provide increasing interest to scientists working on adding functional properties to textile materials. Lam et al176 used plasma pretreatment on cotton fabrics in presence of 1,2,3,4-butanetetracarboxylic acid (BTCA) as a cross-linking agent, and titanium dioxide as a catalyst to obtain enhanced wrinkle resistance property of cotton. Mihailovic and co-workers177 employed RF oxygen and argon plasmas as surface activation methods for the deposition of colloidal TiO2 nanoparticles on polyester fibres. These authors observed that the use of plasma pre-activation and loading with colloidal TiO2 could be successfully employed to impart excellent antibacterial activity against gram-negative bacterium E. coli, UV protection, and good laundering durability of the claimed functionalities. It was also



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shown that discoloration of blueberry juice stain and photodegradation of methylene blue in aqueous solution was the most efficient on polyester fabrics which were exposed to oxygen plasma treatment before loading of colloidal TiO2 nanoparticles (Figure 10). Likewise, anatase TiO2 particles prepared by sol-gel method were applied on polyester fabric treated with low-temperature plasma by Qi et al178 to claim multifunctional finishing properties such as antibacterial activity, colorant decomposition, discoloration of red wine and coffee stains. Moreover, moist CF4 plasma was applied to cellulose fibres by Gorjanc et al,179which proved to improve adsorption of zinc oxide (ZnO) nanoparticles on cellulose. Their study proved that treatment resulted in good ultraviolet protective property of the cellulose fibres. In another research work, Gorjanc et al180 have reported the influence of low-pressure water vapor plasma on introduction of nanosilver into bleached and mercerized cotton fabric. They observed that plasma treatment enhanced nanosilver adsorption thus improved the antimicrobial activity against P. aeruginosa and E.coli. Airoudj et al,181more recently claimed that a new treatment using the deposition of silver nanoparticles on cotton fabrics previously coated with maleic anhydride plasma polymer layer results in development of antibacterial cotton textiles. ATR-FTIR analysis of native cotton had shown characteristics peaks of cellulose however after deposition of maleic anhydride plasma polymer and hydrolysis some new characteristic peaks corresponding to carboxylic and ester groups at around 1730 cm

-1

and 1590-1640 cm-1, respectively appeared in the spectrum. Ilic et al182 introduced a method based on application of low-temperature radio frequency (RF) plasma as a pretreatment method in order to increase the binding efficiency of colloidal silver nanoparticles on the surface of polyester fabrics. It was observed that the pretreated polyester samples showed better antibacterial activity and a good laundering durability, attributed to higher adsorption amount of colloidal silver nanoparticles. Chadeau et al183 evaluated the effects of silver particles (10–100 Å) deposited on cotton and polyester fabrics


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in presence of plasma technology. In their study, antibacterial activity of the finished textiles against L. innocua was measured using standard ISO 20743/2005 methodology and it was found that treated samples had high antimicrobial efficacy against L. innocua. Kostic et al184 prepared silver loaded cotton/polyester fabrics as new antimicrobial materials by modifying cotton/polyester fabrics using DBD technology followed by silver sorption from aqueous silver nitrate solution. They found that the antimicrobial activity of treated fabrics was more effective against Candida albicans than Staphylococcus aureus and Escherichia coli. They claimed high wash durability of the antimicrobial activity. Similarly, Shahidi et al185 demonstrated high antibacterial activity of cotton pre-functionalized by nitrogen plasma in presence of silver absorbed from silver nitrate solution. Vu et al186 applied three different size colloidal silver nanoparticles onto polyamide fabric preactivated by DBD plasma. They used two commercial nanoparticles of size (10and 20 nm) which depicted monodisperse distribution while the third

synthetic ones (50 nm) showed a larger

polydispersity. They reported that all the nanoparticles result in enhanced hydrophobicity besides protect polyamide fabrics against the plasma aging effects. Thorvaldsson et al187 reported coating of textile cellulose microfibre with electrospun cellulose nanofibres followed by modification with fluorine plasma to develop superhydrphobic property which are claimed to have lot of potential textile applications particularly in wound care and tissue engineering. Nawalakhe and co-workers188 developed a novel composite bandage based on deposition of chitosan nanofibres onto atmospheric plasma treated cotton gauze. They found that the composite bandage had higher adhesion, better handling properties, enhanced bioactivity, and moisture management property. 2.4. Effect of UV-irradiation on textile materials Ultraviolet radiation (UVR) is a part of electromagnetic spectrum with wavelength range 100-400nm which is sub dived into UVC (100-280nm), UVB (280-315nm) and UVA (315-



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400nm). UV-C is totally absorbed by the atmosphere and does not reach the earth. The use of UV irradiation in textile coloration offers promise by enhancing dye uptakes, and producing deeper shades without affecting bulk fibre properties. The advantage of UV treatment for textiles is that the chemical changes brought about by their treatment turns out to be restricted in the uppermost layers of substrates thus preventing the fibres from undergoing mechanical loss.60 UV-irradiation introduces carboxylic acid groups into the cotton and may create spaces between fibre linings, possibly due to oxidation of cellulose, thus may enhance the interactions between dye molecules and cellulose functional groups.189, 190 El-Sayed and ElKhatib191 modified wool with ultraviolet light followed by post treatment with an oxidising agent (hydrogen peroxide or sodium monoperoxyphthalate) or a protease enzyme (papain or savinase 16L type EX) and found that the addition of these systems reduced the pilling and shrinkage of wool. About the wool dyeing, Periolatto and co-workers192 observed that wool fabric after irradiation for 5 min at 50 mW/cm2 or 40 s at 900 mW/cm2 can be dyed at 80°C with fast kinetics, total bath exhaustion and good fastness without loss of mechanical properties. Moreover Migliavacca and co-workers193 investigated the UV irradiation of wool fabric as pretreatment for differential dyeing with metal-complex dyes or mixtures of the same with acid dyes. Bhatti and co-workers194 irradiated cellulose fabrics with UV rays followed by dyeing using direct dyes. They compared the results with cellulose fabrics modified by conventional mercerization technique and also dyed with direct dyes. Their study confirmed that UV irradiated cellulosic fabrics had better dye uptakes as compared to the mercerized ones. Likewise Zuber and colleagues195 investigated the dyeing behavior of cellulose fibres in alkaline solutions and under the influence of UV radiation. Several approaches, including effect of UV radiation on the dyeing behaviour of reactive dyes has so far been carried out to improve color strength and fastness properties.196,

197

Lately many researchers have tried to use UV irradiation in natural dyeing to enhance the dye


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fixation on fabrics and to improve depth of shades.

Iqbal and co-workers198 used UV

radiation (245nm, 180 W) for irradiating henna natural dye powder and cotton fabric for one hour. They used different mordants such as copper sulphate and ferrous sulphate for improvement in fastness properties of irradiated dyed cotton fabrics and showed better color strength and fastness properties by pre-irradiated cotton. Adeel and co-workers199 examined the influence of UV irradiation on extraction and dyeing of cotton with Curcuma longa L. They also advised pre- and post-mordanting using copper, iron, and alum mordants to improve fastness properties. They reported that the optimum dyeing conditions for acceptable fastness properties include 55 min dyeing time, 6g/L of sodium sulphate, 1:60 of material-toliquor ratio, and 10 % of alum mordant. Adeel et al200 also treated cotton and barks of Acacia nilotica (Kikar) with UV irradiations for 30, 45, 60, 90 and 120 min. They used different concentrations of mordants such as Cu (copper sulphate), Al (aluminium sulphate), Fe (iron sulphate) and tannic acid to achieve good fastness properties. Parveen et al201 are also among researchers who had studied the effect of UV irradiation on extraction and dyeing of cotton using natural colorants from pomegranate rind. They showed that cotton fabric irradiated with UV and dyed with irradiated pomegranate rind has improved color strength as well as acceptable color fastness to light, washing and rubbing (dry and wet). In addition to their role in textile coloration UV irradiations has also attracted considerable attention in the development of multifunctional textiles. Yuranova and colleagues202 modified polyester- polyamide samples by RF-plasma and vacuum-UV (V-UV) irradiation prior to chemical deposition of Ag-clusters. It was shown that both the treatments were effective in inhibiting the bacterial growth. Ferrero et al203 reported water repellent finishing of cotton by ultraviolet radical curing of silicones and urethane with different formulations. It is worth to mention that UV irradiation can be used as pre-treatment method to anchor nano TiO2 on cotton fabrics to achieve self cleaning property. Ferrero and Periolatto204 also found that



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cotton, silk, and synthetic filter fabrics treated with an acid solution of chitosan in presence of the photo-initiator cured at room temperature by exposure to UV lamp showed substantial increase in antimicrobial activity. Bozzi et al205 discovered that the treatment of bleached cotton and mercerized cotton textile samples by RF-plasma, MW-plasma and UV-irradiation introduces negatively changed functional groups in their structures to deposit nano TiO2 on their surfaces. It was reported that bleached cotton activated by UV irradiation followed by TiO2 deposition from Degussa TiO2 P25 was the most active sample during the discoloration of wine and coffee stains under daylight irradiation while as it case of mercerized cotton TiO2 deposition from a titanium tetra-isopropoxide (TTIP) colloid pre activated with MWplasma depicted favourable discoloration kinetics. The photocatalytic mechanism of TiO2 for discoloration of stains on cotton textiles under UV rays is proposed in Figure 11. The use of carboxylic acids (1, 2,3, 4-butane tetracarboxylic acid (BTCA), maleic acid (MA), succinic acid (SUA), and citric acid (CA) as cross-linking agents for cotton catalyzed with nanotitanium dioxide under UV irradiation and electronic field was studied by Wang and coworkers,206 which claimed to improve their physical properties such as crease recovery and softness properties. Karimi and his co-workers207 applied a process in which nano TiO2 were treated on cotton fabrics after cross-linking was carried with succinic acid under UV irradiation. They found that use of cross-linking improved the self cleaning property of cotton by retaining higher percentage and uniform distribution of nano titania. Alonso and co-workers208 studied the use of citric acid as a cross-linker between chitosan and UV irradiated cellulose fibres in presence of NaH2PO4 as catalyst. They found that incorporation of chitosan was highest in samples previously irradiated with UV and cross liked by citric acid which resulted in their higher antimicrobial activity against fungal and bacterial pathogens. The SEM analysis of the irradiated samples also showed notable morphological changes compared to non-irradiated samples (Figure 12). Kozicki and 24 ACS Paragon Plus Environment

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colleagues209 used screen-printing with printing paste containing silver nitrate exposed to UVC light as an effective antimicrobial finish for cotton textiles. They reported high antibacterial activity of treated samples against Escherichia coli, Bacillus subtilis and Staphylococcus aureus which was maintained for more than 50 washings. Periolatto and coworkers210 studied the influence of UV curing of chitosan on cotton and silk in presence of photo-initiator 2-hydroxy-2-methylphenylpropane-1-one to develop antimicrobial finished fabrics. In addition to cotton and silk, Periolatto et al211 also reported that chitosan UVgrafting is a promising and environmental friendly approach to confer a multifunctional finishing to wool fabrics without affecting the comfort properties. They found that the wool fabrics grafted with 2 % chitosan after an oxidative pre-treatment and 1h impregnation at 50 °C showed 67% reduction of E. coli and 50% of S. aureus. In 2013, Ferrero and coworkers212 explored the influence of UV grafting of chitosan biopolymer on antimicrobial activity of cotton fibre. X-ray photoelectron spectroscopy (XPS), FTIR-ATR analysis, SEM and ninhydrin assays revealed that the chitosan was present on cotton fabric UV-cured with chitosan even after washing and found it highly effective against both E. coli and S. aureus. UV curing is also an alternative to the thermal process to develop aroma finish on textiles in an ecofriendly way. Li et al213 made efforts to study the effect of various finishing conditions such as effects of initiators, UV light sources, and curing speeds on the durability of the encapsulated fragrant finish. The cotton fabric finished with unsaturated polyurethane as an oligomer, tripropylene glycol diacrylate as a monomer, phenyl bis (2, 4, 6-trimethyl benzoyl) phosphine oxide as an initiator, microencapsulated fragrance (45% solid) and cured with iron light at 91 in/min withstood 25 wash cycles retaining its aroma finish. 3. Conclusion and outlook This review articles concentrates on some of the latest approaches based on gamma, ultrasonic, plasma and ultraviolet radiation technologies in producing colored and functional



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textiles for aesthetic, hygienic, and medical applications. High-energy irradiation induced modifications is a promising concept for the introduction of suitable functional groups into fibre structures and for production of

textiles materials with some interesting novel

properties such as self cleaning, insect repellent, fire retardant, UV blocking, water resistant and antimicrobial activity which have recently become popular. Additionally, inclusion of nanomaterials

and use of grafting monomers and cross-linking agents on previously

irradiated textiles have dramatically enhanced their wettability, dyeability, printability, color fastness, and hydrophilicity over the last decade. Irradiation induced modification of textiles seems to be a viable alternative to conventional wet technology and offers full potential for commercialization, besides it may initiate new research opportunities in the development of high value added textiles for various end uses. Acknowledgement: The author Shahid-ul Islam is highly grateful to University Grants Commission, Government of India, for financial support provided through BSR Research Fellowship in Science for Meritorious Students.


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List of Figure Caption Figure 1. Various effects on textile materials using irradiation technologies Figure 2. Some advantages of irradiation technologies over conventional methods Figure 3. Structures of some coloring compounds isolated using gamma irradiation on natural dye powders Figure 4. Structures of some coloring compounds isolated from plants for textile coloration using ultrasound Figure 5. Chemical structure of coloring compounds isolated from lac and cochineal insect dyes (a) Laccaic acid A (b) Laccaic acid B (c) Laccaic acid C (d) Laccaic acid D (e) Laccaic acid E (f) Carminic acid Figure 6. Mechanical properties of the cotton bandage before and after the deposition of MgO nanoparticles, based on the data reported by Perelshtein et al.115 Figure 7. Schematic of plasma reaction of He/1, 3-butadiene with cellulosic textile. Adapted with permission from ref 132. Copyright 2012 Elsevier Figure 8. Deconvoluted XPS C1S and O1S core level spectra of (a, c) untreated wool fibres and (b, d) plasma-treated (1250 W min/m2) wool fibres. Data is based on Oliveira etal.148 Figure 9. FTIR spectra of untreated (black line), Plasma I treated (red line), and Plasma II treated (blue line) cotton nonwoven fabrics in the regions of 1800−800 cm−1 (A, top) and 3500−2600 cm−1 (B, bottom). Data is based on Jinka et al.152 Figure 10. Methylene blue photodegradation by TiO2 nanoparticles on differently modified PES fabrics under UV illumination. Adapted with permission from ref 177. Copyright 2010 American Chemical Society Figure 11. Classical scheme for the production of highly oxidative species by TiO2 under light irradiation with wavelengths

High-Energy Radiation Induced Sustainable Coloration and

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