Indian Patents. 257113:A LYOCELL PERFUMED FIBER AND A METHOD OF MAKING THEREOF

Title of Invention	A LYOCELL PERFUMED FIBER AND A METHOD OF MAKING THEREOF
Abstract	A lyocell fiber having perfume and a method of making thereof is disclosed. Micro-reservoirs are formed in the fibers in which the perfume constituents are embedded.

Full Text	FORM - 2 THE PATENTS ACT, 1970 (39 OF 1970) AND THE PATENTS RULES, 2003 COMPLETE SPECIFICATION (See section 10; rule 13) A LYOCELL PERFUMED FIBER AND A METHOD OF MAKING THEREOF ADITYA BIRLA SCIENCE & TECHNOLOGY CO. LTD. an Indian Company of Aditya Birla Center, 2nd floor, C Wing, S. K. Ahire Marg, Mumbai 400 025, Maharashtra, India THE FOLLOWING SPECIFICATION PARTICULARLY DESCRIBES THE INVENTION AND THE MANNER IN WHICH IT IS TO BE PERFORMED. Field of the invention The present invention relates to textile fibers. Background of the invention The term "fiber" or "textile fiber" means a substance which is capable of being spun into a yarn or made into a fabric by bonding or by interlacing in a variety of methods including weaving, knitting, braiding, felting, twisting, or webbing, and which is the basic structural element of textile products. Fibers are classified on the basis of their length such as short fibers or staple fiber and long fibers or filament fiber. The fibers can also be classified on the basis of their origin such as natural fibers and man-made fibers. The term natural fibers means any fiber that exists as such in the natural state e.g. vegetable fibers or wood fibers. The other type of fibers is obtained from chemical substances. These are called man made fibers. They are rayon, polyester, nylon, acrylic (cashmilon) etc. For centuries, mankind has relied upon various plants and animals to provide raw materials for fabrics and clothing. In recent times, the industrialization and scientific advancement has provided several improved materials having far superior properties, particularly suitable for clothing. Lyocell is a manmade fiber derived from cellulose. Though it is related to rayon, lyocell is obtained by a solvent spinning technique. The solvent spinning technique, which is simpler and more environmentally sound, since it uses a non-toxic solvent chemical that can be recycled in the manufacturing process. 2 It is an extremely strong fabric with industrial uses such as in automotive filters, ropes, abrasive materials, bandages and protective suiting material. It is primarily found in the garment industry, particularly in women's clothing. Lyocell fibers are prepared by following process steps: The raw cellulose is dissolved into heated, pressurized vessel filled with an amine oxide solvent. After soaking for a short time in the solvent, the cellulose forms a clear solution and then it is filtered. The solution is then pumped through spinneret which is pierced with small holes to obtain long strands of fibers. The fibers are then immersed in another dilute solution of amine oxide. This helps to set the fiber strands. Then, they are washed with de-mineralized water. The lyocell fibers are then led to a drying area, where the water is evaporated from it. The strands are led to a finishing area, where the lubricant is applied. The dried, finished fibers are at this stage are called as a tow, which is a large untwisted bundle of continuous length filaments. The bundles of tow are taken to a crimper, a machine which compresses the fiber, giving it texture and bulk. The crimped fiber is then carded by mechanical carders, which perform an action like combing, to separate and order the strands. The carded strands are cut and baled for shipment to a fabric mill. The amine oxide used to dissolve the cellulose and set the fiber after spinning is recovered and re-used in the manufacturing process. From the spun or filament yarn, fabric is formed by knitting or weaving operations. Knitted fabrics can be made by using hooked needles to interlock one or more sets of yarns through a set of loops. The loops may be either loosely or closely constructed, depending on the purpose of the fabric. Knitted fabrics 3 can be used for hosiery, underwear, sweaters, slacks, suits, coats, rugs and other home furnishings. Knitting is performed using either weft or warp processes. Some typical preparations that are involved in the weaving operations are warping, slashing or sizing. Sizing agents are added to the yarn by solution or pad/dry techniques. Differences in raw materials, processing chemicals, fiber diameter, post treatments and blend ratios can be manipulated to produce a fiber having customized properties suitable for desired application. It is often desired that the lyocell fabrics possess typical properties such as thermal stability, ability to retain perfumes, antibacterial properties and the like. These properties are essential in several industrial as well as household applications. There has been a considerable interest in developing such materials. In order to impart various desirable properties to the fabric as mentioned above to the fabric, several additives are added. Such additives include antimicrobial agents, deodorizing agents, antistatic agents, perfumes. Besides such specific additives, generic additives for improving overall quality of the fabric, such as sizing agents, additives for increasing yarn softness and pliability are also added. Prior Art US 7012053 discloses a process for producing treated fabric which involves application of composition, comprising fabric care additive, perfume, color restoring agent and antimicrobial agent by means of spraying, soaking or dipping. Another method of imparting multiple properties to the fabric is disclosed in US 6806213 which involves incorporation of aqueous solution comprising fragrance material, moisturizing agent and surfactant into the fiber. 4 Earlier known processes of incorporating such additives, as reported in the above mentioned patents/applications, mainly involved conventional methods like spraying, encapsulating, solvent spinning the additives on the fabric. However, these methods suffer from several disadvantages which include non¬uniform and improper adhesion of additives onto the fiber material, fading, waning and gradual washing out of the additives over a period of time and which further affects the feel and texture of the fabric. There is thus felt a need for a process of incorporating additives to fabric which overcomes these shortcomings. Objects of the Invention It is an object of this invention to provide perfumed lyocell fibers, wherein at least one perfume constituent is incorporated in the body of the fiber. Another object of this invention is to provide a process of incorporating perfume constituents into lyocell fibers which ensures uniform distribution of the perfume constituent throughout the fiber length. Yet another object of this invention is to provide perfumed lyocell fibers wherein the perfume constituents are retained in the lyocell product over a prolonged period of time. Yet another object of this invention is to provide a process of incorporating perfume constituents to lyocell fibers which does not alter the feel and texture of the fabric. 5 Still another object of this invention is to provide a process of incorporating perfume constituents to lyocell fibers such that inherent properties of the lyocell fibers such as fiber strength, linear density, tenacity, heat resistance, dyeability and drying properties are not altered. Definitions: As used in the present specification, the following words and phrases are generally intended to have the meanings as set forth below, except to the extent that the context in which they are used indicates otherwise. "Non-aqueous phase" means a melted mixture in liquid state which is water insoluble. "Aqueous phase" means substance dissolved in water. "Lyocell Polymer dope" means an intermediate material in the manufacture of lyocell products that is used for preparation of fibers. "Preform mass" means an intermediate material suitable for making fibers. "Perfume constituent for example citrus musk" means a group of compounds which when mixed together provides the scent referred to commercially as citrus musk. Summary of the Invention In accordance with this invention there is provided a perfume lyocell formulation meant for manufacture of lyocell products comprising: 6 • at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation, • at least one water insoluble perfume constituent soluble said solvent, in the range of about 0.001 to 10% of the mass of the formulation, • at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation, • cellulosic pulp in the range of about 3% to 35% of the mass of the formulation • NNMO in the range of about 60 to 80% of the mass of the formulation; and • water in the range of about 0% to 20 % with respect to the mass of the formulation. Typically, the perfume constituent is at least one selected from a group consisting of citrus musk, floral woody, citrus musk woody, fresh bouquet, musk ,floral musk, cedarwood oil, sandalwood oil, lemon oil, orange oil, rose oil, jasmine oil and lavender oil. Typically, the solvent is at least one solvent selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl myristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol, 7 polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins. Typically, the surfactant is at least one non-ionic surfactant selected from a group of non-ionic surfactants consisting of phenoxy like ethoxylated non-ionic surfactants and ethoxylated alkyl alcohol. Typically, the phenoxy ethoxylated non-ionic surfactant is at least one selected from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl), alpha- (nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole ethoxylate), Surfonic N-120(nonylphenol 12-mole ethoxylate), Surfonic N-150 (nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N- 400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14 carbon number alcohol), Igepal CO-630 (nonylphenoxy poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol ethoxylate glycol ether). In accordance with one preferred embodiment of the invention, the HLB value of the surfactant is between 16 and 40. In accordance with one aspect of the invention, the perfume constituent, the solvent and the surfactant are processed to form micro- reservoirs which are embedded into the body of the formulation. 8 Typically, the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm. The invention also extends to a perfume lyocell fiber, yarn and fabric manufactured from a formulation in accordance with this invention. In accordance with this mvention there is also provided a process for preparation of a perfumed lyocell formulation meant for manufacture of lyocell products comprising the following steps : • admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting mixture between 25°C and 95°C to obtain non-aqueous phase ; • dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase; • heating the aqueous-phase; • mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion; • mixing together cellulosic pulp and NNMO to form a slurry; • dispersing the micro-emulsion in the slurry to obtain a preform mass wherein the antimicrobial constituent is embedded in evenly dispersed micro-reservoirs; • vaccumising the preform mass to remove water under 7 to 10 mm of Hg and at temperature over 100°C. Typically, the pH of the aqueous phase is in the range of 7 to 13. 9 Typically, the amount of non-aqueous phase in the micro-emulsion is in the range of 0.1 to 40% of the mass of the micro-emulsion. Typically, the amount of surfactant in the micro-emulsion is in the range of 0.1 to 20% of the mass of the micro-emulsion. Typically, the proportion of perfume constituent in the lyocell product is in the range of 0.001 to 10% with respect to the mass of the lyocell product. Brief Description of the accompanying Drawings: The invention will be described in detail with reference to the accompanying drawings. In the accompanying drawing, Figure 1 illustrates the block diagram showing the method steps involved in the process in accordance with this invention. Figure 2 illustrates the cross-sectional view of perfumed lyocell fibers prepared in accordance with this invention which shows uniform distribution of microreservoirs of perfume constituent entrapped across the length of the fibers. Detailed Description of the Invention A decade of Lyocell technology development has yielded many new opportunities in textile applications due to interesting properties of the solvent spun cellulosic lyocell fibers, especially good mechanical properties and fibrillation resistance. Its versatility and desirable properties provide many advantages, both functional and aesthetic. In terms of performance and properties, lyocell is also friendly to the environment. The resulting fiber, 10 lyocell, is both biodegradable and recyclable Lyocell has strength and durability. Lyocell blends well with other fibers including wool, silk, cotton, linen, nylon, and polyester. It successfully takes many finishes, both functional and those designed to achieve different surface effects and dyes easily. Overall, lyocell is a versatile fiber with many desirable properties. One of the additional desirable properties of Lyocell fibers, which has enormous demand is "perfume activity." In accordance with this invention there is provided a perfumed lyocell formulation meant for manufacture of lyocell products comprising: • at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation, • at least one water insoluble perfume constituent soluble in said solvent, in the range of about 0.001 to 10% of the mass of the formulation, • at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation, • cellulosic pulp in the range of about 3% to 35% of the mass of the formulation • NNMO in the range of about 60 to 80% of the mass of the formulation; and • water in the range of about 0% to 20 % with respect to the mass of the formulation. 11 In accordance with the invention, various perfume constituents from different sources are used. The typical perfume comprises a plurality of individual perfume active compounds, although it can consist essentially of a single perfume ingredient. It is well within the scope of the perfumer of ordinary skill in the art changing ingredients in the perfume component and/or modifying the relative levels of perfume ingredients. In case of synthetic perfume constituents, a perfume constituent is a. composition of one or-more synthetic compounds. Various types of chemical compounds are commonly known for perfumery uses including: phenolic compounds; essential oils; aldehydes; ketones; polycyclic compounds; esters; and alcohols. Many perfume ingredients contain a combination of functional groups and can be categorized under two or more of the above classes. Various plant derived perfume constituents generally include variety of phyto-chemicals along with the principle active phyto-constituent. From the standpoint of the perfumer, it is convenient to consider the perfume ingredients in terms of the type of aroma it imparts rather than the particular chemical class or classes it may fall within. The perfume components herein can be formulated to provide a variety of odor categories: a non-exclusive list includes woody, sweet, citrus, floral, fruity, animal, spice, green, musk, balsamic, chemical, and mint. A variety of exemplary perfume ingredients are described below for several of the commonly used odor categories, long with their representative (but not necessarily exclusive) chemical categories. Woody perfume ingredients include cedarwood oil (essential oil), guaicwood oil (essential oil), gamma ionone (ketone), sandalwood oil (essential oil), and methyl cedrylone (ketone). Sweet perfume ingredients include coumarin 12 (ketone), vanillin (4 hydroxy-3methoxy benzaldehyde) (aldehyde), ethyl maltol (Alcohol), phenyl acetaldehyde (aldehyde), heliotropin (aldehyde), acetophenone (ketone), and dihydrocoumarin (ketone). Citrus perfume ingredients include orange oil (essential oil), lemon oil (essential oil), citral (aldehyde), beta methyl naphthyl ketone (ketone), terpinyl acetate (ester), nonyl aldehyde (aldehyde), terpineol (alcohol), and dihydromyrcenol (alcohol). Floral perfume ingredients include a variety of floral subcategories, such as rose, lavender, jasmin, and muguet. Rose perfume ingredients include geranyl acetate (ester), geraniol (alcohol), citronelyl acetate (ester), phenyl ethyl alcohol (alcohol), alpha damascone (ketone), beta damascone (ketone), geranium oil (essential oil), and natural rose oil (essential oil). Lavender perfume ingredients include dihydro terpinyl acetate (ester), ethyl hexyl ketone (ketone), lavandin (essential oil), lavender (essential oil), tetra hydro linalool (alcohol), linalool (alcohol), and linalyl acetate (ester). Jasmin perfume ingredients include benzyl acetate (ester), butyl cinnamic aldehyde (aldehyde), methyl benzoate (ester), natural jasmin oil (essential oil), methyl dihydro jasmonate (ester). Muguet perfume ingredients include cycalmen aldehyde (aldehyde), benzyl salycilate (ester), hydroxycitronellol (alcohol), citronellyl oxyacetaldehyde (aldehyde), and hydroxy aldehyde (aldehyde). Fruity perfume ingredients include ethyl-2-methyl butyrate (ester), allyl cyclohexane propionate (ester), amyl acetate (ester), ethyl acetate 13 (ester), gamma decalactone (ketone), octaiactone (ketone), undecalactone (aldehyde), ethyl aceto acetate (ester), benzaldehyde (aldehyde). Animal perfume ingredients include methyl phenyl acetate (ester), indol (2,3, benzpyrrole) (phenolic), creosol (phenolic), iso butyl quinolin (phenolic), and androstenol (phenolic). Spice perfume ingredients include anisic aldehyde (aldehyde), anise (essential oil), clove oil (essential oil), eugenol (phenolic), iso eugenol (phenolic), thymol (phenolic), anethol (phenolic), cinnamic alcohol (alcohol), and cinnamic aldehyde (aldehyde). Green perfume ingredients include beta gamma nexenol (alcohol) brom styrol (alcohol), dimethyl benzyl carbinol (alcohol), methyl heptine cart onate (ester), cis-3-hexenyl acetate (ester), and galbanum oil (essential oil). Musk perfume ingredients often also function as fixatives. Examples of musk include glaxolide (phenol), cyclopentadecanolide (phenol), musk ketone (ketone), ambrettolide (phenol), tonalid (phenol), and ethylene brassylate (ester). Balsamic perfume ingredients include fir balsam (essential oil, peru balsam (essential oil), and benzoin resinoid (essential oil). Mint perfume ingredients include laevo carvone (ketone), menthol (alcohol), methyl salicylate (ester), peppermint oil (essential oil), spearmint oil (essential oil), eucalyptus (essential oil), anisyl acetate (ester), methyl chavicol (alcohol). Nonionic Surfactant 14 Chemical perfume ingredients include benzyl alcohol (alcohol), diproplene glycol (alcohol), ethanol (alcohol), and benzyl benzoate (ester) , Andrane, Cedramber, Decyl methyl ether, Galaxolid, Grisalv, Indolarome-soli, Orange flower ether, Ozofleu, Phenafleu, Tobacaro, Paracresyl methyl Ether, Karana, Cyclogalbanat, Piconi, Iso-cyclemone, Iso E supe, Celestolide-soli, Fleuramon,, ihydroisojasmon, Isojasmon, Tonali, Methyl Ionone , Dulcinyl-soli, Acetanisol, Vetikon, Undecylenic Aldehyd, lilia, Vanilli, Cinnamic Alcoho, Iso-Eugeno, Tetra-Hydro Geranio, Calone 10 % DE, Dihydro-isojasmon, Galaxolide, Karanal 10% DE, Yara Yara (Nerolin) , Decyl methyl ether, Ethyl Methyl Phenyl Glycidate, Para-Cresyl Phenyl acetate, Undecalactone, Clonal IFF Preferred plant derived perfume compositions are provided herein below : Rose oil : beta-damascenone, beta-damascone, beta-ionone and rose oxide. Lavender oil : linalool and linalyl acetate. Orange oil: d-limonene. Jasmine oil : benzyl acetate, linalool, benzyl alcohol, indole, benzyl benzoate, cis-jasmone, geraniol and methyl anthranilate. Sandalwood oil : santalols, santene, nor-tricycloekasantalene and a- and β- santalenes, santenol and teresantalol. Cedarwood oil : p-methyl-5-3- tetrahydroacetophenone, p-methyl acetophenone, cis- and trans- atlantones, a- and p-himalchenes, ar- dihydroturmerone and himachalol. The perfume constituent impart peculiar pleasant aroma or fragrance to the fibers and ultimately to the fabric or garments made from these fibers. 15 In accordance with this invention, only non-aqueous solvent is used which is typically selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl niyristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol, polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins. Preferably, paraffin wax either alone or in combination with stearyl alcohol is used as the non-aqueous solvent. In accordance with this invention a water soluble non-ionic surfactant/co- surfactant is used. Typically, the non-ionic surfactant is selected from a group consisting of phenoxy ethoxylated non-ionic surfactants and ethoxylated alkyl alcohol. Typically, the phenoxy ethoxylated non-ionic surfactant is at least one selected from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl), alpha- (nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole ethoxylate), Surfonic N-120(nonylphenol 12-mole ethoxylate) , Surfonic N-150 (nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N- 400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14 carbon number alcohol), Igepal CO-630 (nonylphenoxy 16 poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol ethoxylate glycol ether). The non-ionic surfactant is selected such that the lipophilic portion of the non-ionic surfactant is compatible with the perfume constituent and the surfactant forms oil in water micro-emulsion. Surfactants with HLB values within the range of 9 to 40 are used. Preferably, non-ionic surfactants with HLB values more than 13 are used. In accordance with one preferred embodiment of the invention, the HLB value of the surfactant is between 16 and 40. In accordance with one aspect of the invention, the perfume constituent, the solvent and the surfactant are processed to form micro-reservoirs which are embedded into the body of the formulation. The perfumed lyocell contains uniformly dispersed micro-reservoirs throughout the body of the fibers. The micro-reservoirs are discrete, nano-sized structures without any definite geometrical shape. Typically, the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm. The invention also extends to a perfume lyocell fiber, yarn and fabric manufactured from a formulation in accordance with this invention. 17 In accordance with this invention there is also provided a process for preparation of a perfume lyocell formulation meant for manufacture of lyocell products comprising the following steps : • admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting admixture upto 95 C to obtain non-aqueous phase ; • dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase; • heating the aqueous-phase; • mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion; • mixing together cellulosic pulp and NNMO to form a slurry; • dispersing the micro-emulsion in the slurry to obtain a preform mass wherein the antimicrobial constituent is embedded in evenly dispersed micro-reservoirs; • vaccumising the preform mass to remove water under 7 to 10 mm of Hg and at temperature over 100°C to obtain the formulation. Typically, the pH of the aqueous phase is in the range of 7 to 13. Typically, the amount of non-aqueous phase in the micro-emulsion is in the range of 0.1 to 40% of the mass of the micro-emulsion. Typically, the amount of surfactant in the micro-emulsion is in the range of 0.1 to 20% of the mass of the micro-emulsion. 18 Typically, the proportion of perfume constituent in the lyocell product is in the range of 0.001 to 10% with respect to the mass of the lyocell product. Before arriving at the optimum concentration of the surfactant to be used, cloud point of the aqueous phase is determined. Furthermore, alkalinity of the aqueous phase matches with that of the viscous polymer dope thereby avoiding any drastic change in the alkalinity during the emulsification and homogenization step. Typically, the melted non-aqueous phase containing perfume constituent in a non-aqueous solvent along with aqueous phase containing surfactants is emulsified using high speed mixers such as Ultraturrex or a mechanical emulsifier; a colloid mill; a high pressure homogenizer and an ultrasonic emulsifier to form a micro-emulsion. The micro-emulsion may contain further additional perfume constituents, if desired. The active ingredients are released from the micro-reservoir into the lyocell matrix. The structure of micro-reservoir, lyocell and surrounding conditions determine the release rate of the perfume constituent. The molecules of the volatile perfume constituents migrate from micro-reservoirs to the surrounding primarily by diffusion. The perfume constituent is released from the matrix in a controlled release manner. Conventional method for in manufacture of lyocell involves following major steps : 19 Step 1. Creating a solvent solution from wood pulp The wood pulp is obtained from a variety of sources, such as wood chips or even large rolls of paper that have been finely shredded, is the basic starting material for manufacture of lyocell fibers. In case of manufacture of lyocell no further chemical treatment of the wood pulp is needed thereby making the process environment friendly. The wood pulp solution is produced in a straight solvation process by dissolving wood pulp at high temperatures and pressure in a recyclable non-toxic organic solvent solution of amine oxide, particularly N-methylmorpholine N-oxide,(NNMO). Lyocell is manufactured by a "closed loop" spinning process which conserves energy and water. Step 2. Spinning lyocell fiber from the solvent solution Before being formed into fibers, the lyocell polymer dope, is in a thick liquid state. In the spinning process this liquid is forced through a spinneret, which resembles a large shower head. The clear, viscous resultant solution is filtered and extruded into an aqueous bath of dilute amine oxide, and coagulated into fiber form. Step 3. Washing lyocell fiber to remove solvents. The fiber is then washed before it is dried and twisted or spun into yarns, which are woven or knitted into fabrics and garments. 20 Step 4. Drying fiber and producing yarns. When the filament dries or solidifies, it forms what is called a continuous filament fiber. Many continuous filaments of specific thicknesses collected in a large bundle called a "tow". A tow may contain over a million continuous filaments. The tow bundle is then crimped, is then mechanically cut into staple fibers, usually ranging in length from 1 to 6-1/2 inches, depending how they are to be used. Strands of continuous filament fibers are then twisted together to form a continuous filament yarn, which is then woven or knit into fabric. Step 5. Finishing to produce lyocell fabric. The fabric is treated with an enzyme that attacks cellulose fibers. Home laundry detergents containing such enzymes are also used for treatment of the fabric for better finishing purposes. This enzyme dissolves the split-end hairs from the fiber surface. The fiber is then washed and agitated again. The resulting fabric is similar in texture and drape to sueded silk or sueded rayon found in fashion apparel. Fabrics processed this way can usually be machine washed and line dried successfully. Alternatively, the filaments so obtained are stretched to straighten out the fibers which are further blended using standard equipment. The blended fibers are laid in to a web followed by Consolidation of the web to obtain Non-woven Lyocell Fabric. 21 The lyocell product made from the formulation in accordance with this invention contains uniformly dispersed micro-reservoirs throughout the mass which is shown in Fig. 2. A typical perfumed lyocell fiber as obtained by the process of this invention contains the releasable perfume constituent entrapped in the form of pockets. Said pockets are uniformly distributed throughout the length of the fiber. Upon microscopic examination, perfume constituent enriched lyocell fiber shows uniform distribution of pockets along the length of the lyocell fiber as shown in Fig. 2. The resultant perfumed lyocell fabric is tested. Linear Density (Denier) of the lyocell Fibers is determined by using standard ASTM Test Method (D 1577). The denier of the standard lyocell fiber (lyocell fiber without any perfume constituents) and perfume enriched lyocell fiber remains the same. Thus addition of perfume does not change the linear density of the lyocell fibers. Tensile strength and Young's modulus of lyocell fiber sample is tested on an Instron tensile testing machine as per the ASTM CI557-03 procedure at ambient temperature. Visual appearance of the perfume enriched fiber is evaluated by methods as prescribed in AATCC 124. As far as parameters like % Loss in Dry Tenacity and % loss in dry elongation are concerned, these remain the same in the perfume enriched lyocell fiber and the standard fiber. Incorporation of perfume constituent in accordance with this invention does not affect the visual appearance of the fiber. 22 Feel of the fiber: The perfume enriched lyocell fiber as prepared in accordance with this invention offers the same feel effect as is observed in case of plain lyocell fiber without any perfume constituent (Also referred as standard). Another important concern in textile industry is dye-ability of the fabric, which is tested by comparing the dyeability of the perfume constituent enriched fabric and the standard lyocell fabric. Dyeability of the perfume enriched lyocell fibers as prepared in accordance with this invention remains the same as that of the standard lyocell fiber. Perfume retention test: Perfumed lyocell fabric before and after washes is tested for aroma or fragrance by using an expert human panel. Fragrance of the perfumed lyocell fibers as prepared in accordance with this invention remains the same even after repeatedly washing the fabric and exposing it to sunlight and / or varying temperatures. The invention will now be described with the help of the following non-limiting examples. Examples Example 1 Example 1A- Preparation of micro emulsion Stearyl alcohol (225 gms) was heated until it melts and (50gm) of citrus musk was admixed to form a molten mixture (275gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. 23 The aqueous phase (553 gm) and the mixture (275 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (828 gm ). Example 1 B- Preparation fiber and fabric 1000 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a slurry (4250gm).The micro-emulsion as prepared in Example 1A was evenly dispersed in the slurry to obtain a preform mass (5000 gm). The homogenized preform mass was vaccumisied to remove water under 10 mm of Hg and at temperature 110 °C ,was further spun in a spin bath of dilute amine oxide, and coagulated into fiber form. The fiber was then washed before it was dried and spun into a fabric. The lyocell fiber thus obtained contained micro-reservoirs having the entrapped releasable antimicrobial constituents. Although the micro reservoirs did not have any specific shape or size, they were found to be uniformly distributed throughout the body of the fiber. Example 2 Example 2 A- Preparation of micro emulsion Myristyl alcohol (225 gms) was heated until it melts and (60gm) of floral woody was admixed to form a molten mixture (275gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (275 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (828 gm ). 24 Example 2 B Preparation of fiber 990 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a slurry (4250gm).The micro-emulsion as prepared in Example 2A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 3 Example3 A Preparation of antimicrobial formulation Polyvinyl laurate (200 gms) and cetyl alcohol ( 25 gm) was heated until it melts and (lOOgm) of woody musk was admixed to form a molten mixture (325gm). Surforvic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm). Example 3 B- Preparation of fiber 922 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a slurry (4200gm).The micro-emulsion as prepared in Example 3A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 4 Example 4 A Preparation of antimicrobial formulation 25 Polyvinyl laurate (250 gms) and cetyl alcohol (25 gm) was heated until it melts and (50 gm) of fresh bouquet was admixed to form a molten mixture (325gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm). Example 4 B- Preparation fiber and fabric 1400 gm of cellulosic pulp and 2800 gm of NNMO solvent were mixed to form a slurry (4200gm).The micro-emulsion as prepared in Example 4A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 5 Example 5A Preparation of antimicrobial formulation Polypropylene glycol (100 gm) and paraffin wax (175 gm) were heated until it melts and (50 gm) of floral musk was admixed to form a molten mixture (325gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm). Example 5 B- Preparation fiber and fabric 1200 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form a slurry (4200gm).The micro-emulsion as prepared in Example 5A was evenly 26 dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 6 Example 6 A Preparation of antimicrobial formulation Stearyl alcohol (200gm) and polyethylene(HDPE) (lOOgm) were melted together to form a molten liquid. To this (200gm) of citrus musk was added to form a molten mixture (500gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm). Example 6 B- Preparation fiber and fabric 947 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 6A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 7 Example 7 A Preparation of antimicrobial formulation Polyvinyl stearate (150 gm) and paraffin wax (lOOgm) were melted together to form a molten liquid. To this citrus musk woody (150 gm) was added to form a molten mixture (400 gm). - 27 Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The-aqueous phase (553 gm) and the mixture (400 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (953 gm). Example 7 B- Preparation fiber and fabric 1047 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 7A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 8 Example 8 A Preparation of antimicrobial formulation Polypentane glutarate (300 gm) was melted to form a molten liquid- To this (lOOgm) floral woody was added to form a mixture (400 gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (400 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (953 gm). Example 8 B 1547 gm of cellulosic pulp and 2500 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 8A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. 28 Example 9 Example 9 A Preparation of antimicrobial formulation Stearyl alcohol ( 250 gm) and paraffin wax (200 gm) were melted together to form a molten liquid. To this (50gm) of fresh bouquet was added to form a mixture (500 gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm) of aqueous phase. The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm). Example 9 B 1147 gm of cellulosic pulp and 2900 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 8A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Example 10 Example 10 A Preparation of micro emulsion Stearyl alcohol (150 gm) and polyvinyl laurate (150gm) were melted together to form a molten liquid. To this molten liquid, (200gm) of lavender oil was added to form a mixture (500gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm) of aqueous phase. The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm). 29 Example 10 B 1347 gm of cellulosic pulp and 2700 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 10 A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1. Testing procedures: The perfumed lyocell products as prepared in the above examples (1 to 10) were tested by using following test procedures: 1) Linear Density (Denier) of the lyocell Fibers was determined by using standard ASTM Test Method (D 1577). The denier of the standard lyocell fiber (without any perfume constituents) and anti-microbial lyocell fibers as prepared in accordance with example IB was found to be uniform(l .5 denier) irrespective of the type and quantity of the perfume constituent. 2) Tensile strength and Young's modulus of lyocell fiber samples were tested on an Instron tensile testing machine as per the ASTM C1557-03 procedure at ambient temperature. 3) Emulsion stability: The stability of micro-emulsions as prepared in the above examples, was evaluated by keeping the same under observation in measuring cylinders for 3 days. During this period no phase separation was observed. 4) Feel of the fabric: The lyocell fabrics as prepared in the above examples and standard fabric (lyocell fabric without perfume constituents), were randomly given to twenty subjects and they were asked to evaluate the texture and feel of the fiber. The test fiber material was interchanged several 30 times amongst the human subjects. Collective results as submitted by the human subjects confirmed that nobody could distinguish between thewith perfumed lyocell fabrics prepared in accordance with the Examples provided above and the standard fabric. 5) Dyeability: The perfumed lyocell fabrics as prepared in the above examples and the standard fabric as described above were dyed uniformly with reactive dyes. No noticeable difference as to the Dyeability of the two respective lyocell fabrics, with and without perfume constituent was reported. 6) Visual appearance of the perfumed lyocell fiber was evaluated by methods as prescribed in AATCC 124. As far as parameters like % Loss in Dry Tenacity and % loss in dry elongation are concerned, these remained the same( 7) Perfume retension test: Twenty pieces of standard size 20cmX20cm cut out from the freshly prepared lyocell fiber as prepared in accordance with example IB. Another set of Twenty pieces of the same size cut out of from the same fiber were subjected to 20 hot water washes with the intermittent drying period of 2 firs. The drying was carried out in natural sunlight at temperature within the range of 25 to 45°C. The specimens so prepared were randomly distributed to human subjects for testing the aroma of the specimen. The specimen was interchanged amongst the subjects. No noticeable difference in odor of the two respective lyocell fiber specimens was reported and therefore it is 31 concluded that the lyocell fiber specimen retained the perfume additive even after exposure to varying conditions. While considerable emphasis has been placed herein on the specific steps of the preferred embodiment, it will be appreciated that many alterations can be made and that many modifications can be made in the preferred embodiment without departing from the principles of the invention. These and other changes in the preferred embodiment as well as other embodiments of the invention will be apparent to those skilled in the art from the disclosure herein, whereby it is to be distinctly understood that the foregoing descriptive matter is to be interpreted merely as illustrative of the invention and not as a limitation. 32 We Claim: 1. A perfumed lyocell formulation meant for manufacture of lyocell products comprising : • at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation, • at least one water insoluble perfume constituent soluble said solvent, in the range of about 0.001 to 10% of the mass of the formulation, • at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation, • cellulosic pulp in the range of about 3% to 35% of the mass of the formulation • NNMO in the range of about 60 to 80% of the mass of the formulation; and • water in the range of about 0% to 20 % with respect to the mass of the formulation. 2. A formulation as claimed in claim 1, wherein the perfume constituent is at least one selected from a group consisting of citrus musk, floral woody, citrus musk woody, fresh bouquet, musk , floral musk , lavender oil, jasmine oil, rose oil, cedarwood oil, sandalwood oil, orange oil and lemon oil. 3. A formulation as claimed in claim 1, wherein the solvent is at least one solvent selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene 33 glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl myristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol, polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins. 4. A formulation as claimed in claim 1, wherein the surfactant is at least one non-ionic surfactant selected from a group of non-ionic surfactants consisting of phenoxy like ethoxylated non-ionic surfactants and ethoxylated alkyl alcohol. 5. A formulation as claimed in claim 8, wherein the phenoxy like ethoxylated non-ionic surfactant is at least one selected from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl), alpha- (nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole ethoxylate) , Surfonic N-120(nonylphenol 12-mole ethoxylate) , Surfonic N-150 (nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N-400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14 carbon number alcohol), Igepal CO-630 (nonylphenoxy poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol ethoxylate glycol ether). 34 6. A formulation as claimed in claim 1, wherein the preferred HLB value of the surfactant is between 16 and 40. 7. A formulation as claimed in claim 1, wherein the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm. 8. A perfumed lyocell fiber manufactured from a formulation as claimed in claim 1. 9. A perfumed lyocell yarn manufactured from a formulation as claimed in claim 1. 10.A perfumed lyocell fabric manufactured from a formulation as claimed in claim 1. 11. A process of preparation of a perfumed lyocell formulation meant for manufacture of lyocell products comprising the following steps : • admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting mixture between 25°C and 95°C to obtain non-aqueous phase ; • dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase; • heating the aqueous-phase; • mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion; 35 mixing together cellulosic pulp and NNMO to form a slurry; dispersing the micro-emulsion in the slurry to obtain a preform mass wherein the antimicrobial constituent is embedded in evenly dispersed micro-reservoirs; vaccumising the preform mass to remove water under 7 to 10 mm of Hg and at temperature over 100°C to obtain the formulation. ,rd Dated this 3ra day of July, 2008. Mohan Dewan of R. K. Dewan and Co. Applicants' Patent Attorney 36

Full Text

FORM - 2
THE PATENTS ACT, 1970
(39 OF 1970)
AND
THE PATENTS RULES, 2003
COMPLETE SPECIFICATION
(See section 10; rule 13)
A LYOCELL PERFUMED FIBER AND A METHOD OF

MAKING THEREOF
ADITYA BIRLA SCIENCE & TECHNOLOGY CO. LTD.
an Indian Company of Aditya Birla Center, 2nd floor, C Wing, S. K. Ahire Marg, Mumbai 400 025,
Maharashtra, India

THE FOLLOWING SPECIFICATION PARTICULARLY DESCRIBES THE INVENTION AND THE MANNER IN WHICH IT IS TO BE PERFORMED.

Field of the invention
The present invention relates to textile fibers.
Background of the invention
The term "fiber" or "textile fiber" means a substance which is capable of being spun into a yarn or made into a fabric by bonding or by interlacing in a variety of methods including weaving, knitting, braiding, felting, twisting, or webbing, and which is the basic structural element of textile products.
Fibers are classified on the basis of their length such as short fibers or staple fiber and long fibers or filament fiber. The fibers can also be classified on the basis of their origin such as natural fibers and man-made fibers. The term natural fibers means any fiber that exists as such in the natural state e.g. vegetable fibers or wood fibers. The other type of fibers is obtained from chemical substances. These are called man made fibers. They are rayon, polyester, nylon, acrylic (cashmilon) etc.
For centuries, mankind has relied upon various plants and animals to provide raw materials for fabrics and clothing. In recent times, the industrialization and scientific advancement has provided several improved materials having far superior properties, particularly suitable for clothing.
Lyocell is a manmade fiber derived from cellulose. Though it is related to rayon, lyocell is obtained by a solvent spinning technique. The solvent spinning technique, which is simpler and more environmentally sound, since it uses a non-toxic solvent chemical that can be recycled in the manufacturing process.
2

It is an extremely strong fabric with industrial uses such as in automotive filters,
ropes, abrasive materials, bandages and protective suiting material. It is
primarily found in the garment industry, particularly in women's clothing.
Lyocell fibers are prepared by following process steps:
The raw cellulose is dissolved into heated, pressurized vessel filled with an
amine oxide solvent.
After soaking for a short time in the solvent, the cellulose forms a clear solution
and then it is filtered.
The solution is then pumped through spinneret which is pierced with small holes
to obtain long strands of fibers. The fibers are then immersed in another dilute
solution of amine oxide. This helps to set the fiber strands. Then, they are
washed with de-mineralized water.
The lyocell fibers are then led to a drying area, where the water is evaporated
from it. The strands are led to a finishing area, where the lubricant is applied.
The dried, finished fibers are at this stage are called as a tow, which is a large
untwisted bundle of continuous length filaments. The bundles of tow are taken
to a crimper, a machine which compresses the fiber, giving it texture and bulk.
The crimped fiber is then carded by mechanical carders, which perform an
action like combing, to separate and order the strands. The carded strands are cut
and baled for shipment to a fabric mill.
The amine oxide used to dissolve the cellulose and set the fiber after spinning is
recovered and re-used in the manufacturing process.
From the spun or filament yarn, fabric is formed by knitting or weaving operations. Knitted fabrics can be made by using hooked needles to interlock one or more sets of yarns through a set of loops. The loops may be either loosely or closely constructed, depending on the purpose of the fabric. Knitted fabrics
3

can be used for hosiery, underwear, sweaters, slacks, suits, coats, rugs and other home furnishings. Knitting is performed using either weft or warp processes.
Some typical preparations that are involved in the weaving operations are warping, slashing or sizing. Sizing agents are added to the yarn by solution or pad/dry techniques. Differences in raw materials, processing chemicals, fiber diameter, post treatments and blend ratios can be manipulated to produce a fiber having customized properties suitable for desired application. It is often desired that the lyocell fabrics possess typical properties such as thermal stability, ability to retain perfumes, antibacterial properties and the like. These properties are essential in several industrial as well as household applications. There has been a considerable interest in developing such materials. In order to impart various desirable properties to the fabric as mentioned above to the fabric, several additives are added. Such additives include antimicrobial agents, deodorizing agents, antistatic agents, perfumes. Besides such specific additives, generic additives for improving overall quality of the fabric, such as sizing agents, additives for increasing yarn softness and pliability are also added.
Prior Art
US 7012053 discloses a process for producing treated fabric which involves application of composition, comprising fabric care additive, perfume, color restoring agent and antimicrobial agent by means of spraying, soaking or dipping.
Another method of imparting multiple properties to the fabric is disclosed in US 6806213 which involves incorporation of aqueous solution comprising fragrance material, moisturizing agent and surfactant into the fiber.
4

Earlier known processes of incorporating such additives, as reported in the above mentioned patents/applications, mainly involved conventional methods like spraying, encapsulating, solvent spinning the additives on the fabric. However, these methods suffer from several disadvantages which include non¬uniform and improper adhesion of additives onto the fiber material, fading, waning and gradual washing out of the additives over a period of time and which further affects the feel and texture of the fabric.
There is thus felt a need for a process of incorporating additives to fabric which overcomes these shortcomings.
Objects of the Invention
It is an object of this invention to provide perfumed lyocell fibers, wherein at least one perfume constituent is incorporated in the body of the fiber.
Another object of this invention is to provide a process of incorporating perfume constituents into lyocell fibers which ensures uniform distribution of the perfume constituent throughout the fiber length.
Yet another object of this invention is to provide perfumed lyocell fibers wherein the perfume constituents are retained in the lyocell product over a prolonged period of time.
Yet another object of this invention is to provide a process of incorporating perfume constituents to lyocell fibers which does not alter the feel and texture of the fabric.
5

Still another object of this invention is to provide a process of incorporating perfume constituents to lyocell fibers such that inherent properties of the lyocell fibers such as fiber strength, linear density, tenacity, heat resistance, dyeability and drying properties are not altered.
Definitions:
As used in the present specification, the following words and phrases are generally intended to have the meanings as set forth below, except to the extent that the context in which they are used indicates otherwise.
"Non-aqueous phase" means a melted mixture in liquid state which is water
insoluble.
"Aqueous phase" means substance dissolved in water.
"Lyocell Polymer dope" means an intermediate material in the manufacture of
lyocell products that is used for preparation of fibers.
"Preform mass" means an intermediate material suitable for making fibers.
"Perfume constituent for example citrus musk" means a group of
compounds which when mixed together provides the scent referred to
commercially as citrus musk.
Summary of the Invention
In accordance with this invention there is provided a perfume lyocell formulation meant for manufacture of lyocell products comprising:
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• at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation,
• at least one water insoluble perfume constituent soluble said solvent, in the range of about 0.001 to 10% of the mass of the formulation,
• at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation,
• cellulosic pulp in the range of about 3% to 35% of the mass of the formulation
• NNMO in the range of about 60 to 80% of the mass of the formulation; and
• water in the range of about 0% to 20 % with respect to the mass of the formulation.
Typically, the perfume constituent is at least one selected from a group consisting of citrus musk, floral woody, citrus musk woody, fresh bouquet, musk ,floral musk, cedarwood oil, sandalwood oil, lemon oil, orange oil, rose oil, jasmine oil and lavender oil.
Typically, the solvent is at least one solvent selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl myristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol,
7

polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins.
Typically, the surfactant is at least one non-ionic surfactant selected from a group of non-ionic surfactants consisting of phenoxy like ethoxylated non-ionic surfactants and ethoxylated alkyl alcohol.
Typically, the phenoxy ethoxylated non-ionic surfactant is at least one selected
from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl), alpha-
(nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole
ethoxylate), Surfonic N-120(nonylphenol 12-mole ethoxylate), Surfonic N-150
(nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole
ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N-
400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene
ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14
carbon number alcohol), Igepal CO-630 (nonylphenoxy
poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol
ethoxylate glycol ether).
In accordance with one preferred embodiment of the invention, the HLB value of the surfactant is between 16 and 40.
In accordance with one aspect of the invention, the perfume constituent, the solvent and the surfactant are processed to form micro- reservoirs which are embedded into the body of the formulation.
8

Typically, the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm.
The invention also extends to a perfume lyocell fiber, yarn and fabric manufactured from a formulation in accordance with this invention.
In accordance with this mvention there is also provided a process for preparation of a perfumed lyocell formulation meant for manufacture of lyocell products comprising the following steps :
• admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting mixture between 25°C and 95°C to obtain non-aqueous phase ;
• dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase;
• heating the aqueous-phase;
• mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion;
• mixing together cellulosic pulp and NNMO to form a slurry;
• dispersing the micro-emulsion in the slurry to obtain a preform mass wherein the antimicrobial constituent is embedded in evenly dispersed micro-reservoirs;
• vaccumising the preform mass to remove water under 7 to 10 mm of Hg and at temperature over 100°C.
Typically, the pH of the aqueous phase is in the range of 7 to 13.
9

Typically, the amount of non-aqueous phase in the micro-emulsion is in the range of 0.1 to 40% of the mass of the micro-emulsion.
Typically, the amount of surfactant in the micro-emulsion is in the range of 0.1 to 20% of the mass of the micro-emulsion.
Typically, the proportion of perfume constituent in the lyocell product is in the range of 0.001 to 10% with respect to the mass of the lyocell product.
Brief Description of the accompanying Drawings:
The invention will be described in detail with reference to the accompanying drawings.
In the accompanying drawing, Figure 1 illustrates the block diagram showing the method steps involved in the process in accordance with this invention.
Figure 2 illustrates the cross-sectional view of perfumed lyocell fibers prepared in accordance with this invention which shows uniform distribution of microreservoirs of perfume constituent entrapped across the length of the fibers.
Detailed Description of the Invention
A decade of Lyocell technology development has yielded many new opportunities in textile applications due to interesting properties of the solvent spun cellulosic lyocell fibers, especially good mechanical properties and fibrillation resistance. Its versatility and desirable properties provide many advantages, both functional and aesthetic. In terms of performance and properties, lyocell is also friendly to the environment. The resulting fiber,
10

lyocell, is both biodegradable and recyclable Lyocell has strength and durability. Lyocell blends well with other fibers including wool, silk, cotton, linen, nylon, and polyester. It successfully takes many finishes, both functional and those designed to achieve different surface effects and dyes easily. Overall, lyocell is a versatile fiber with many desirable properties.
One of the additional desirable properties of Lyocell fibers, which has enormous demand is "perfume activity."
In accordance with this invention there is provided a perfumed lyocell formulation meant for manufacture of lyocell products comprising:
• at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation,
• at least one water insoluble perfume constituent soluble in said solvent, in the range of about 0.001 to 10% of the mass of the formulation,
• at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation,
• cellulosic pulp in the range of about 3% to 35% of the mass of the formulation
• NNMO in the range of about 60 to 80% of the mass of the formulation; and
• water in the range of about 0% to 20 % with respect to the mass of the formulation.
11

In accordance with the invention, various perfume constituents from different sources are used. The typical perfume comprises a plurality of individual perfume active compounds, although it can consist essentially of a single perfume ingredient. It is well within the scope of the perfumer of ordinary skill in the art changing ingredients in the perfume component and/or modifying the relative levels of perfume ingredients.
In case of synthetic perfume constituents, a perfume constituent is a. composition of one or-more synthetic compounds. Various types of chemical compounds are commonly known for perfumery uses including: phenolic compounds; essential oils; aldehydes; ketones; polycyclic compounds; esters; and alcohols. Many perfume ingredients contain a combination of functional groups and can be categorized under two or more of the above classes. Various plant derived perfume constituents generally include variety of phyto-chemicals along with the principle active phyto-constituent.
From the standpoint of the perfumer, it is convenient to consider the perfume ingredients in terms of the type of aroma it imparts rather than the particular chemical class or classes it may fall within. The perfume components herein can be formulated to provide a variety of odor categories: a non-exclusive list includes woody, sweet, citrus, floral, fruity, animal, spice, green, musk, balsamic, chemical, and mint. A variety of exemplary perfume ingredients are described below for several of the commonly used odor categories, long with their representative (but not necessarily exclusive) chemical categories.
Woody perfume ingredients include cedarwood oil (essential oil), guaicwood oil (essential oil), gamma ionone (ketone), sandalwood oil (essential oil), and methyl cedrylone (ketone). Sweet perfume ingredients include coumarin
12

(ketone), vanillin (4 hydroxy-3methoxy benzaldehyde) (aldehyde), ethyl maltol (Alcohol), phenyl acetaldehyde (aldehyde), heliotropin (aldehyde), acetophenone (ketone), and dihydrocoumarin (ketone).
Citrus perfume ingredients include orange oil (essential oil), lemon oil (essential oil), citral (aldehyde), beta methyl naphthyl ketone (ketone), terpinyl acetate (ester), nonyl aldehyde (aldehyde), terpineol (alcohol), and dihydromyrcenol (alcohol).
Floral perfume ingredients include a variety of floral subcategories, such as rose, lavender, jasmin, and muguet. Rose perfume ingredients include geranyl acetate (ester), geraniol (alcohol), citronelyl acetate (ester), phenyl ethyl alcohol (alcohol), alpha damascone (ketone), beta damascone (ketone), geranium oil (essential oil), and natural rose oil (essential oil). Lavender perfume ingredients include dihydro terpinyl acetate (ester), ethyl hexyl ketone (ketone), lavandin (essential oil), lavender (essential oil), tetra hydro linalool (alcohol), linalool (alcohol), and linalyl acetate (ester). Jasmin perfume ingredients include benzyl acetate (ester), butyl cinnamic aldehyde
(aldehyde), methyl benzoate (ester), natural jasmin oil (essential oil), methyl dihydro jasmonate (ester). Muguet perfume ingredients include cycalmen aldehyde (aldehyde), benzyl salycilate (ester), hydroxycitronellol (alcohol), citronellyl oxyacetaldehyde (aldehyde), and hydroxy aldehyde (aldehyde).
Fruity perfume ingredients include ethyl-2-methyl butyrate (ester), allyl cyclohexane propionate (ester), amyl acetate (ester), ethyl acetate
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(ester), gamma decalactone (ketone), octaiactone (ketone), undecalactone (aldehyde), ethyl aceto acetate (ester), benzaldehyde (aldehyde).
Animal perfume ingredients include methyl phenyl acetate (ester), indol (2,3, benzpyrrole) (phenolic), creosol (phenolic), iso butyl quinolin (phenolic), and androstenol (phenolic).
Spice perfume ingredients include anisic aldehyde (aldehyde), anise (essential oil), clove oil (essential oil), eugenol (phenolic), iso eugenol (phenolic), thymol (phenolic), anethol (phenolic), cinnamic alcohol (alcohol), and cinnamic aldehyde (aldehyde).
Green perfume ingredients include beta gamma nexenol (alcohol) brom styrol (alcohol), dimethyl benzyl carbinol (alcohol), methyl heptine cart onate (ester), cis-3-hexenyl acetate (ester), and galbanum oil (essential oil).
Musk perfume ingredients often also function as fixatives. Examples of musk include glaxolide (phenol), cyclopentadecanolide (phenol), musk ketone (ketone), ambrettolide (phenol), tonalid (phenol), and ethylene brassylate (ester).
Balsamic perfume ingredients include fir balsam (essential oil, peru balsam (essential oil), and benzoin resinoid (essential oil).
Mint perfume ingredients include laevo carvone (ketone), menthol (alcohol), methyl salicylate (ester), peppermint oil (essential oil), spearmint oil (essential oil), eucalyptus (essential oil), anisyl acetate (ester), methyl chavicol (alcohol). Nonionic Surfactant
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Chemical perfume ingredients include benzyl alcohol (alcohol), diproplene glycol (alcohol), ethanol (alcohol), and benzyl benzoate (ester) , Andrane, Cedramber, Decyl methyl ether, Galaxolid, Grisalv, Indolarome-soli, Orange flower ether, Ozofleu, Phenafleu, Tobacaro, Paracresyl methyl Ether, Karana, Cyclogalbanat, Piconi, Iso-cyclemone, Iso E supe, Celestolide-soli, Fleuramon,, ihydroisojasmon, Isojasmon, Tonali, Methyl Ionone , Dulcinyl-soli, Acetanisol, Vetikon, Undecylenic Aldehyd, lilia, Vanilli, Cinnamic Alcoho, Iso-Eugeno, Tetra-Hydro Geranio, Calone 10 % DE, Dihydro-isojasmon, Galaxolide, Karanal 10% DE, Yara Yara (Nerolin) , Decyl methyl ether, Ethyl Methyl Phenyl Glycidate, Para-Cresyl Phenyl acetate, Undecalactone, Clonal IFF
Preferred plant derived perfume compositions are provided herein below :
Rose oil : beta-damascenone, beta-damascone, beta-ionone and rose oxide.
Lavender oil : linalool and linalyl acetate.
Orange oil: d-limonene.
Jasmine oil : benzyl acetate, linalool, benzyl alcohol, indole, benzyl benzoate,
cis-jasmone, geraniol and methyl anthranilate.
Sandalwood oil : santalols, santene, nor-tricycloekasantalene and a- and β-
santalenes, santenol and teresantalol.
Cedarwood oil : p-methyl-5-3- tetrahydroacetophenone, p-methyl
acetophenone, cis- and trans- atlantones, a- and p-himalchenes, ar-
dihydroturmerone and himachalol.
The perfume constituent impart peculiar pleasant aroma or fragrance to the fibers and ultimately to the fabric or garments made from these fibers.
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In accordance with this invention, only non-aqueous solvent is used which is typically selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl niyristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol, polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins.
Preferably, paraffin wax either alone or in combination with stearyl alcohol is used as the non-aqueous solvent.
In accordance with this invention a water soluble non-ionic surfactant/co-
surfactant is used. Typically, the non-ionic surfactant is selected from a group
consisting of phenoxy ethoxylated non-ionic surfactants and ethoxylated alkyl
alcohol. Typically, the phenoxy ethoxylated non-ionic surfactant is at least one
selected from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl),
alpha- (nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole
ethoxylate), Surfonic N-120(nonylphenol 12-mole ethoxylate) , Surfonic N-150
(nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole
ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N-
400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene
ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14
carbon number alcohol), Igepal CO-630 (nonylphenoxy
16

poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol
ethoxylate glycol ether).
The non-ionic surfactant is selected such that the lipophilic portion of the non-ionic surfactant is compatible with the perfume constituent and the surfactant forms oil in water micro-emulsion. Surfactants with HLB values within the range of 9 to 40 are used. Preferably, non-ionic surfactants with HLB values more than 13 are used.
In accordance with one preferred embodiment of the invention, the HLB value of the surfactant is between 16 and 40.
In accordance with one aspect of the invention, the perfume constituent, the solvent and the surfactant are processed to form micro-reservoirs which are embedded into the body of the formulation. The perfumed lyocell contains uniformly dispersed micro-reservoirs throughout the body of the fibers. The micro-reservoirs are discrete, nano-sized structures without any definite geometrical shape.
Typically, the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm.
The invention also extends to a perfume lyocell fiber, yarn and fabric manufactured from a formulation in accordance with this invention.
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In accordance with this invention there is also provided a process for preparation of a perfume lyocell formulation meant for manufacture of lyocell products comprising the following steps :
• admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting admixture upto 95 C to obtain non-aqueous phase ;
• dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase;
• heating the aqueous-phase;
• mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion;
• mixing together cellulosic pulp and NNMO to form a slurry;
• dispersing the micro-emulsion in the slurry to obtain a preform mass wherein the antimicrobial constituent is embedded in evenly dispersed micro-reservoirs;
• vaccumising the preform mass to remove water under 7 to 10 mm of Hg and at temperature over 100°C to obtain the formulation.
Typically, the pH of the aqueous phase is in the range of 7 to 13.
Typically, the amount of non-aqueous phase in the micro-emulsion is in the range of 0.1 to 40% of the mass of the micro-emulsion.
Typically, the amount of surfactant in the micro-emulsion is in the range of 0.1 to 20% of the mass of the micro-emulsion.
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Typically, the proportion of perfume constituent in the lyocell product is in the range of 0.001 to 10% with respect to the mass of the lyocell product.
Before arriving at the optimum concentration of the surfactant to be used, cloud point of the aqueous phase is determined. Furthermore, alkalinity of the aqueous phase matches with that of the viscous polymer dope thereby avoiding any drastic change in the alkalinity during the emulsification and homogenization step.
Typically, the melted non-aqueous phase containing perfume constituent in a non-aqueous solvent along with aqueous phase containing surfactants is emulsified using high speed mixers such as Ultraturrex or a mechanical emulsifier; a colloid mill; a high pressure homogenizer and an ultrasonic emulsifier to form a micro-emulsion. The micro-emulsion may contain further additional perfume constituents, if desired.
The active ingredients are released from the micro-reservoir into the lyocell matrix. The structure of micro-reservoir, lyocell and surrounding conditions determine the release rate of the perfume constituent. The molecules of the volatile perfume constituents migrate from micro-reservoirs to the surrounding primarily by diffusion. The perfume constituent is released from the matrix in a controlled release manner.
Conventional method for in manufacture of lyocell involves following major steps :
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Step 1. Creating a solvent solution from wood pulp
The wood pulp is obtained from a variety of sources, such as wood chips or even large rolls of paper that have been finely shredded, is the basic starting material for manufacture of lyocell fibers. In case of manufacture of lyocell no further chemical treatment of the wood pulp is needed thereby making the process environment friendly.
The wood pulp solution is produced in a straight solvation process by dissolving wood pulp at high temperatures and pressure in a recyclable non-toxic organic solvent solution of amine oxide, particularly N-methylmorpholine N-oxide,(NNMO).
Lyocell is manufactured by a "closed loop" spinning process which conserves energy and water.
Step 2. Spinning lyocell fiber from the solvent solution
Before being formed into fibers, the lyocell polymer dope, is in a thick liquid state. In the spinning process this liquid is forced through a spinneret, which resembles a large shower head.
The clear, viscous resultant solution is filtered and extruded into an aqueous bath of dilute amine oxide, and coagulated into fiber form.
Step 3. Washing lyocell fiber to remove solvents.
The fiber is then washed before it is dried and twisted or spun into yarns, which are woven or knitted into fabrics and garments.
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Step 4. Drying fiber and producing yarns.
When the filament dries or solidifies, it forms what is called a continuous filament fiber. Many continuous filaments of specific thicknesses collected in a large bundle called a "tow". A tow may contain over a million continuous filaments. The tow bundle is then crimped, is then mechanically cut into staple fibers, usually ranging in length from 1 to 6-1/2 inches, depending how they are to be used.
Strands of continuous filament fibers are then twisted together to form a continuous filament yarn, which is then woven or knit into fabric.
Step 5. Finishing to produce lyocell fabric.
The fabric is treated with an enzyme that attacks cellulose fibers. Home laundry detergents containing such enzymes are also used for treatment of the fabric for better finishing purposes. This enzyme dissolves the split-end hairs from the fiber surface. The fiber is then washed and agitated again. The resulting fabric is similar in texture and drape to sueded silk or sueded rayon found in fashion apparel. Fabrics processed this way can usually be machine washed and line dried successfully.
Alternatively, the filaments so obtained are stretched to straighten out the fibers which are further blended using standard equipment. The blended fibers are laid in to a web followed by Consolidation of the web to obtain Non-woven Lyocell Fabric.
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The lyocell product made from the formulation in accordance with this invention contains uniformly dispersed micro-reservoirs throughout the mass which is shown in Fig. 2.
A typical perfumed lyocell fiber as obtained by the process of this invention contains the releasable perfume constituent entrapped in the form of pockets. Said pockets are uniformly distributed throughout the length of the fiber. Upon microscopic examination, perfume constituent enriched lyocell fiber shows uniform distribution of pockets along the length of the lyocell fiber as shown in Fig. 2.
The resultant perfumed lyocell fabric is tested. Linear Density (Denier) of the lyocell Fibers is determined by using standard ASTM Test Method (D 1577). The denier of the standard lyocell fiber (lyocell fiber without any perfume constituents) and perfume enriched lyocell fiber remains the same. Thus addition of perfume does not change the linear density of the lyocell fibers. Tensile strength and Young's modulus of lyocell fiber sample is tested on an Instron tensile testing machine as per the ASTM CI557-03 procedure at ambient temperature.
Visual appearance of the perfume enriched fiber is evaluated by methods as prescribed in AATCC 124. As far as parameters like % Loss in Dry Tenacity and % loss in dry elongation are concerned, these remain the same in the perfume enriched lyocell fiber and the standard fiber. Incorporation of perfume constituent in accordance with this invention does not affect the visual appearance of the fiber.
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Feel of the fiber: The perfume enriched lyocell fiber as prepared in accordance with this invention offers the same feel effect as is observed in case of plain lyocell fiber without any perfume constituent (Also referred as standard). Another important concern in textile industry is dye-ability of the fabric, which is tested by comparing the dyeability of the perfume constituent enriched fabric and the standard lyocell fabric. Dyeability of the perfume enriched lyocell fibers as prepared in accordance with this invention remains the same as that of the standard lyocell fiber.
Perfume retention test:
Perfumed lyocell fabric before and after washes is tested for aroma or fragrance by using an expert human panel. Fragrance of the perfumed lyocell fibers as prepared in accordance with this invention remains the same even after repeatedly washing the fabric and exposing it to sunlight and / or varying temperatures.
The invention will now be described with the help of the following non-limiting examples.
Examples
Example 1
Example 1A- Preparation of micro emulsion
Stearyl alcohol (225 gms) was heated until it melts and (50gm) of citrus musk
was admixed to form a molten mixture (275gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
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The aqueous phase (553 gm) and the mixture (275 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (828 gm ).
Example 1 B- Preparation fiber and fabric
1000 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a slurry (4250gm).The micro-emulsion as prepared in Example 1A was evenly dispersed in the slurry to obtain a preform mass (5000 gm). The homogenized preform mass was vaccumisied to remove water under 10 mm of Hg and at temperature 110 °C ,was further spun in a spin bath of dilute amine oxide, and coagulated into fiber form. The fiber was then washed before it was dried and spun into a fabric.
The lyocell fiber thus obtained contained micro-reservoirs having the entrapped releasable antimicrobial constituents. Although the micro reservoirs did not have any specific shape or size, they were found to be uniformly distributed throughout the body of the fiber.
Example 2
Example 2 A- Preparation of micro emulsion
Myristyl alcohol (225 gms) was heated until it melts and (60gm) of floral woody
was admixed to form a molten mixture (275gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
The aqueous phase (553 gm) and the mixture (275 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (828 gm ).
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Example 2 B
Preparation of fiber
990 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a
slurry (4250gm).The micro-emulsion as prepared in Example 2A was evenly
dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into
fiber as described in example 1.
Example 3
Example3 A
Preparation of antimicrobial formulation
Polyvinyl laurate (200 gms) and cetyl alcohol ( 25 gm) was heated until it melts
and (lOOgm) of woody musk was admixed to form a molten mixture (325gm).
Surforvic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm).
Example 3 B- Preparation of fiber
922 gm of cellulosic pulp and 3200 gm of NNMO solvent were mixed to form a slurry (4200gm).The micro-emulsion as prepared in Example 3A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 4
Example 4 A
Preparation of antimicrobial formulation
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Polyvinyl laurate (250 gms) and cetyl alcohol (25 gm) was heated until it melts and (50 gm) of fresh bouquet was admixed to form a molten mixture (325gm). Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm).
Example 4 B- Preparation fiber and fabric
1400 gm of cellulosic pulp and 2800 gm of NNMO solvent were mixed to form a slurry (4200gm).The micro-emulsion as prepared in Example 4A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 5
Example 5A
Preparation of antimicrobial formulation
Polypropylene glycol (100 gm) and paraffin wax (175 gm) were heated until it
melts and (50 gm) of floral musk was admixed to form a molten mixture
(325gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
The aqueous phase (553 gm) and the mixture (325 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (878 gm).
Example 5 B- Preparation fiber and fabric
1200 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form
a slurry (4200gm).The micro-emulsion as prepared in Example 5A was evenly
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dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 6
Example 6 A
Preparation of antimicrobial formulation
Stearyl alcohol (200gm) and polyethylene(HDPE) (lOOgm) were melted
together to form a molten liquid. To this (200gm) of citrus musk was added to
form a molten mixture (500gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm).
Example 6 B- Preparation fiber and fabric
947 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 6A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 7
Example 7 A
Preparation of antimicrobial formulation
Polyvinyl stearate (150 gm) and paraffin wax (lOOgm) were melted together to
form a molten liquid. To this citrus musk woody (150 gm) was added to form a
molten mixture (400 gm).
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Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase. The-aqueous phase (553 gm) and the mixture (400 gm) were homogenized in a high speed mixer (Ultraturrex) to obtain a micro-emulsion (953 gm).
Example 7 B- Preparation fiber and fabric
1047 gm of cellulosic pulp and 3000 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 7A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 8
Example 8 A
Preparation of antimicrobial formulation
Polypentane glutarate (300 gm) was melted to form a molten liquid- To this
(lOOgm) floral woody was added to form a mixture (400 gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm)of aqueous phase.
The aqueous phase (553 gm) and the mixture (400 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (953 gm).
Example 8 B
1547 gm of cellulosic pulp and 2500 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 8A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
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Example 9
Example 9 A
Preparation of antimicrobial formulation
Stearyl alcohol ( 250 gm) and paraffin wax (200 gm) were melted together to
form a molten liquid. To this (50gm) of fresh bouquet was added to form a
mixture (500 gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm) of aqueous phase.
The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm).
Example 9 B
1147 gm of cellulosic pulp and 2900 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 8A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Example 10
Example 10 A
Preparation of micro emulsion
Stearyl alcohol (150 gm) and polyvinyl laurate (150gm) were melted together
to form a molten liquid. To this molten liquid, (200gm) of lavender oil was
added to form a mixture (500gm).
Surfonic N-400 nonylphenol 40-mole ethoxylate (surfactant) (28 gm ) was
dissolved and stirred in water (525 ml) to obtain (553 gm) of aqueous phase.
The aqueous phase (553 gm) and the mixture (500 gm) were homogenized in a
high speed mixer (Ultraturrex) to obtain a micro-emulsion (1053 gm).
29

Example 10 B
1347 gm of cellulosic pulp and 2700 gm of NNMO solvent were mixed to form a slurry (3947gm).The micro-emulsion as prepared in Example 10 A was evenly dispersed in the slurry to obtain a preform mass (5000 gm) and was spun into fiber as described in example 1.
Testing procedures:
The perfumed lyocell products as prepared in the above examples (1 to 10) were tested by using following test procedures:
1) Linear Density (Denier) of the lyocell Fibers was determined by using
standard ASTM Test Method (D 1577).
The denier of the standard lyocell fiber (without any perfume constituents) and anti-microbial lyocell fibers as prepared in accordance with example IB was found to be uniform(l .5 denier) irrespective of the type and quantity of the perfume constituent.
2) Tensile strength and Young's modulus of lyocell fiber samples were tested on an Instron tensile testing machine as per the ASTM C1557-03 procedure at ambient temperature.
3) Emulsion stability: The stability of micro-emulsions as prepared in the above examples, was evaluated by keeping the same under observation in measuring cylinders for 3 days. During this period no phase separation was observed.
4) Feel of the fabric: The lyocell fabrics as prepared in the above examples and standard fabric (lyocell fabric without perfume constituents), were randomly given to twenty subjects and they were asked to evaluate the texture and feel of the fiber. The test fiber material was interchanged several
30

times amongst the human subjects. Collective results as submitted by the human subjects confirmed that nobody could distinguish between thewith perfumed lyocell fabrics prepared in accordance with the Examples provided above and the standard fabric.
5) Dyeability: The perfumed lyocell fabrics as prepared in the above examples and the standard fabric as described above were dyed uniformly with reactive dyes. No noticeable difference as to the Dyeability of the two respective lyocell fabrics, with and without perfume constituent was reported.
6) Visual appearance of the perfumed lyocell fiber was evaluated by methods as prescribed in AATCC 124. As far as parameters like % Loss in Dry Tenacity and % loss in dry elongation are concerned, these remained the same( 7) Perfume retension test:
Twenty pieces of standard size 20cmX20cm cut out from the freshly prepared lyocell fiber as prepared in accordance with example IB. Another set of Twenty pieces of the same size cut out of from the same fiber were subjected to 20 hot water washes with the intermittent drying period of 2 firs. The drying was carried out in natural sunlight at temperature within the range of 25 to 45°C. The specimens so prepared were randomly distributed to human subjects for testing the aroma of the specimen. The specimen was interchanged amongst the subjects. No noticeable difference in odor of the two respective lyocell fiber specimens was reported and therefore it is
31

concluded that the lyocell fiber specimen retained the perfume additive even after exposure to varying conditions.
While considerable emphasis has been placed herein on the specific steps of the preferred embodiment, it will be appreciated that many alterations can be made and that many modifications can be made in the preferred embodiment without departing from the principles of the invention. These and other changes in the preferred embodiment as well as other embodiments of the invention will be apparent to those skilled in the art from the disclosure herein, whereby it is to be distinctly understood that the foregoing descriptive matter is to be interpreted merely as illustrative of the invention and not as a limitation.
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We Claim:
1. A perfumed lyocell formulation meant for manufacture of lyocell products
comprising :
• at least one non-aqueous solvent in the range of about 0.01 to 20% of the mass of the formulation,
• at least one water insoluble perfume constituent soluble said solvent, in the range of about 0.001 to 10% of the mass of the formulation,
• at least one water soluble non-cationic surfactant having HLB value in the range of 9 to 40, in the range of range of 0.001 to 10% of the mass of the formulation,
• cellulosic pulp in the range of about 3% to 35% of the mass of the formulation
• NNMO in the range of about 60 to 80% of the mass of the formulation; and
• water in the range of about 0% to 20 % with respect to the mass of the formulation.

2. A formulation as claimed in claim 1, wherein the perfume constituent is at least one selected from a group consisting of citrus musk, floral woody, citrus musk woody, fresh bouquet, musk , floral musk , lavender oil, jasmine oil, rose oil, cedarwood oil, sandalwood oil, orange oil and lemon oil.
3. A formulation as claimed in claim 1, wherein the solvent is at least one solvent selected from a group of solvents consisting of C10-C44 alkanes (paraffinic hydrocarbons), polyethylene, polypropylene, polypropylene
33

glycol, polytetramethylene glycol, polypropylene malonate, polyneopentyl glycol sebacate, polypentane glutarate, polyvinyl myristate, polyvinyl stearate, polyvinyl laurate, polyhexadecyl methacrylate, polyoctadecyl methacrylate, polyethylene oxides, polyethylene glycols, Arachidyl alcohol, behenyl alcohol, Selachyl alcohol, chimimyl alcohol, polyesters, di-iso decyl phthalate, benzyl alcohol, C4 -C30 aliphatic alcohols ,C4 -C30 saturated hydrocarbons, C4 -C30 monounsaturated hydrocarbons, natural oils and mineral oil paraffins.
4. A formulation as claimed in claim 1, wherein the surfactant is at least one non-ionic surfactant selected from a group of non-ionic surfactants consisting of phenoxy like ethoxylated non-ionic surfactants and ethoxylated alkyl alcohol.
5. A formulation as claimed in claim 8, wherein the phenoxy like ethoxylated non-ionic surfactant is at least one selected from a group consisting of Surfonic N-95(Poly (oxy-1, 2-ethanediyl), alpha- (nonyl phenyl)-omega-hydroxyl-glycol ether) ( nonylphenol 9.5-mole ethoxylate) , Surfonic N-120(nonylphenol 12-mole ethoxylate) , Surfonic N-150 (nonylphenol 15-mole ethoxylate), Surfonic N-200 (nonylphenol 20-mole ethoxylate) , Surfonic N-300( nonylphenol 30-mole ethoxylate) , Surfonic N-400 nonylphenol 40-mole ethoxylate, Surfonic LF-7 (Alkyl polyoxyalkylene ether) , Surfonic LF-17 (ethoxylated and propoxylated linear primary 12-14 carbon number alcohol), Igepal CO-630 (nonylphenoxy poly(ethyleneoxy)ethanol,branched), Surfonic DNP-40 (dinonylphenol ethoxylate glycol ether).
34

6. A formulation as claimed in claim 1, wherein the preferred HLB value of the surfactant is between 16 and 40.
7. A formulation as claimed in claim 1, wherein the average mean size of the micro-reservoir is in the range of 5 nm to 2000 nm.
8. A perfumed lyocell fiber manufactured from a formulation as claimed in claim 1.
9. A perfumed lyocell yarn manufactured from a formulation as claimed in claim 1.
10.A perfumed lyocell fabric manufactured from a formulation as claimed in claim 1.
11. A process of preparation of a perfumed lyocell formulation meant for manufacture of lyocell products comprising the following steps :
• admixing a water-insoluble perfume constituent with a non-aqueous solvent followed by heating the resulting mixture between 25°C and 95°C to obtain non-aqueous phase ;
• dissolving and stirring a surfactant, optionally with a co-surfactant, in water to obtain an aqueous phase;
• heating the aqueous-phase;
• mixing the aqueous phase with the non-aqueous phase in the liquid state to form a admixture and homogenizing to obtain a micro-emulsion;
35

mixing together cellulosic pulp and NNMO to form a slurry;
dispersing the micro-emulsion in the slurry to obtain a preform mass
wherein the antimicrobial constituent is embedded in evenly dispersed
micro-reservoirs;
vaccumising the preform mass to remove water under 7 to 10 mm of
Hg and at temperature over 100°C to obtain the formulation.

,rd
Dated this 3ra day of July, 2008.

Mohan Dewan
of R. K. Dewan and Co.
Applicants' Patent Attorney

36

Documents:

1396-mum-2008 abstract.pdf

1396-mum-2008 claims.pdf

1396-mum-2008 correspondence.pdf

1396-mum-2008 description(complete).pdf

1396-mum-2008 drawing.pdf

1396-mum-2008 form 1.pdf

1396-mum-2008 form 2(titel page).pdf

1396-mum-2008 form 2.pdf

1396-mum-2008 form 3.pdf

1396-mum-2008-abstract.doc

1396-MUM-2008-ANNEXURE TO FORM 3(26-9-2012).pdf

1396-MUM-2008-CLAIMS(AMENDED)-(26-9-2012).pdf

1396-mum-2008-claims.doc

1396-MUM-2008-CORRESPONDENCE(13-04-2010).pdf

1396-mum-2008-correspondence(18-7-2008).pdf

1396-MUM-2008-CORRESPONDENCE(24-7-2009).pdf

1396-MUM-2008-CORRESPONDENCE(6-8-2013).pdf

1396-mum-2008-description(complete).doc

1396-MUM-2008-EP DOCUMENT(26-9-2012).pdf

1396-mum-2008-form 1(18-7-2008).pdf

1396-MUM-2008-FORM 1(6-8-2013).pdf

1396-MUM-2008-FORM 13(6-8-2013).pdf

1396-MUM-2008-FORM 18(24-7-2009).pdf

1396-mum-2008-form 2.doc

1396-MUM-2008-FORM 26(26-9-2012).pdf

1396-MUM-2008-FORM 3(13-04-2010).pdf

1396-mum-2008-form 3(3-7-2008).pdf

1396-MUM-2008-MARKED COPY(26-9-2012).pdf

1396-MUM-2008-REPLY TO EXAMINATION REPORT(26-9-2012).pdf

1396-MUM-2008-SPECIFICATION(AMENDED)-(26-9-2012).pdf

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Patent Number

257113

Indian Patent Application Number

1396/MUM/2008

PG Journal Number

36/2013

Publication Date

06-Sep-2013

Grant Date

03-Sep-2013

Date of Filing

03-Jul-2008

Name of Patentee

ADITYA BIRLA SCIENCE & TECHNOLOGY CO. LTD.

Applicant Address

ADITYA BIRLA CENTRE, 2ND FLOOR, C WING, S.K. AHIRE MARG, MUMBAI,

Inventors:

#	Inventor's Name	Inventor's Address
1	LODHA PREETI	ADITYA BIRLA CENTRE, 2ND FLOOR, C WING, S.K. AHIRE MARG, MUMBAI-400025,
2	KAPOOR BIR	ADITYA BIRLE CENTRE, 2ND FLOOR, C WING, S.K. AHIRE MARG, MUMBAI-400025,
3	MAHAJAN TUSHAR	ADITYA BIRLA CENTRE, 2ND FLOOR, C WING, S.K. AHIRE MARG, MUMBAI-400025,

PCT International Classification Number

C08K5/03

PCT International Application Number

N/A

PCT International Filing date

PCT Conventions:

#	PCT Application Number	Date of Convention	Priority Country
1	NIL	1900-01-01	India