Abstract:
An improved cosmetic composition comprises at least one cosmetically effective ingredient and water, where at least a potion of the water has been replaced by a distillate of a green plant juice. The distillate is obtained from a green plant juice, produced by squeezing green plants, by evaporation of the green plant juice to cause a concentration increase of the green plant juice.

Description:
CROSS REFERENCE TO RELATED APPLICATION 
     This application is a continuation of application Ser. No. 09/563,921, filed May 4, 2000 now abn. 
    
    
     BACKGROUND OF THE INVENTION 
     1. Field of the Invention 
     The present invention relates to cosmetic compositions which normally contain purified or distilled water wherein the water has been at least partially replaced by a distillate of a green plant juice. More particularly, the present invention is directed to cosmetic compositions containing at least one cosmetically effective ingredient and a distillate of a green plant juice; and methods of producing the same. 
     2. Description of the Prior Art 
     Fresh raw edible green plants are very important foodstuffs for the maintenance of health, but they involve problems concerning edibility, e.g., in that they are tough and hard to digest. In order to solve these problems, various foodstuffs comprising green plant juice squeezed from a fresh raw edible green plant or its dry powder have been proposed in the prior art. 
     In the preparation of such dry powders, a large amount of liquid is removed from the green plant juice and then discarded as a waste material. 
     The present invention provides a use for this by-product liquid. 
     BRIEF SUMMARY OF THE INVENTION 
     It is an object of the present invention to utilize an otherwise discarded by-product of the manufacture of a dry powder of green plant juice. 
     It is a further object of the present invention to provide a cosmetic composition having reduced requirements for preservative materials. 
     It is a still further object of the present invention to provide a process for producing a cosmetic composition having reduced requirements for preservative materials. 
     These objects of the invention, and others that will become apparent upon reading the disclosure of this invention, are achieved by the provision of an improved cosmetic composition comprising at least one cosmetically effective ingredient and water, wherein the improvement is the replacement of at least a portion of the water by a distillate of a green plant juice. 
     Additionally, the present invention provides an improved process for producing a cosmetic composition comprising mixing at least one cosmetically effective ingredient and water, wherein the improvement is the replacement of at least a portion of the water by a distillate of a green plant juice. 
    
    
     BRIEF DESCRIPTION OF THE DRAWINGS 
     FIG. 1 is a graph illustrating the antioxidant activity of the distillate of green plant juice as tested in Example 2. 
    
    
     DETAILED DESCRIPTION OF THE INVENTION 
     The presently contemplated distillate of a green plant juice is obtained as a by-product of the production of dry powder of green plant juice squeezed from a fresh raw edible green plant. 
     In this production process, the leaves and/or stems, preferably leaves and stems, of young green plants are harvested; the harvested materials are washed with water; the washed materials are squeezed to collect a green plant juice; the green plant juice is concentrated (producing the distillate of a green plant juice used in this invention and a concentrate); the concentrate is spray-dried into a powder; and the powder is granulated and packed into jars. 
     The green plants which are used as starting materials in the present invention are preferably edible green plants and these include not only cultivated edible plants having green leaves or stems, but also edible wild grasses and herbs having green leaves and stems; plants having green leaves and stems which are not usually eaten, such as fruit, vegetables, root crops, cereals and fruit trees; green edible algae; and the like. Specific examples thereof include green leaves of barley and wheat, spinach, lettuce, cabbage, Chinese cabbage, Japanese cabbage, cucumber, bitter melon, pimento, carrot leaves, radish leaves, parsley, celery, “ashitaba” ( Angelica keiskei  (Miq.) koidz.), comfrey leaves, green leaves of grasses, (e.g., alfalfa, clover and kale), striped bamboo leaves, persimmon leaves, pine needles, spirulina, chlorella, “wakame seaweed” ( Undaria pinnatifida  (Harvey) Suringar) and green laver. These plants may be used alone or in combination of two or more. 
     Among the foregoing green plants, cereals such as barley, wheat, rye, oats, pearl barley, corn, millet and Italian ryegrass are preferred. Of these, barley (in particular, its leaves and stems before maturation) is most preferred. 
     It is desirable to treat these green plants while they are as fresh as possible. Where stored plants are used, it is preferable that they have been subjected to proper measures for the prevention of discoloration and deterioration, such as inert gas storage, cold storage, deaerated and dehydrated storage, or treatment with sulfur dioxide or a sulfite salt. A green plant used as the starting material is thoroughly washed to remove all of the matter adhering thereto, preferably such washing is effected using room temperature water (with no detergents being involved); sterilized with a germicide (e.g., hypochlorous acid), as desired; further washed thoroughly with water; and, optionally, cut to pieces of appropriate size. When cut to pieces, the plant may be soaked in a dilute aqueous solution of sodium chloride (e.g., a 0.1-2% aqueous solution of sodium chloride) and cut therein. Moreover, at any stage of this pretreatment, the plant may be subjected to a blanching treatment at a temperature of 100° C. to 140° C. under atmospheric pressure (or under sub-atmospheric or super-atmospheric pressure in some cases) for about 2 to 10 seconds and then cooled rapidly. This treatment serves to inactivate enzymes which may cause undesirable discoloration or deterioration of green plants (e.g., chlorophyllase, peroxidases and polyphenol oxidase). 
     After the green plant is pre-treated in the above-described manner, juice is squeezed therefrom. The squeezing can readily be carried out according to any conventionally known method, for example, by the combined use of a mechanical disintegration means (such as a mixer or juicer) and a solid-liquid separation means (such as a centrifuge or a filter apparatus). Water may be added to the green plant material prior to the squeezing in order to facilitate handling of the green plant material. After the squeezing, the pH of the resulting green juice may be adjusted to a pH of 6.2 to 9.5, preferably 6.5 to 8.5, more preferably, about 6.5 to 7.5, by use of a base. 
     Bases which can be used for the above-described pH adjustment include hydroxides, carbonates and bicarbonates of alkali metals and alkaline earth metals, such as sodium hydroxide, calcium hydroxide, magnesium hydroxide, sodium carbonate, potassium carbonate, calcium carbonate and sodium bicarbonate; ammonium hydroxide; glutamic acid salts such as calcium glutamate; and kelp extract. 
     At any stage following the separation of the green juice and preceding the drying treatment, the green plant juice may be subjected to a flash heating treatment for decomposing or inactivating undesirable enzymes which will participate in discoloration or deterioration, and also destroying bacteria which may be present therein. This treatment may be carried out under atmospheric, sub-atmospheric or super-atmospheric pressure, using a heating temperature of 90° C. to 150° C. and a treating time of about 180 to 2 seconds. After such a treatment, it is desirable to cool the juice rapidly, particularly to a temperature of 10° C. or below. 
     As described previously, the green plant juice having undergone the pH adjustment is spray-dried or freeze-dried, preferably spray-dried, as soon as possible. The spray-drying or freeze-drying may be carried out according to any conventionally known method. 
     For example, in the case of spray drying, hot spray drying using hot air at about 120° C. to 200° C., preferably 140° C. to 170° C., or cold spray drying using air dried with a suitable desiccant, e.g., lithium chloride, may be employed. In the case of freeze drying, treating conditions such as drying plate temperature of 40° C. to 50° C. and a vacuum of the order of 1.0 to 0.01 mmHg are usually employed. 
     The concentration of the green plant juice (i.e. solids content) used in the drying step should be in the range of about 1.5 to 30% and preferably as high as possible within those limits. In order to concentrate the green juice to this end, a continuous thin-film concentrator or a vacuum distillation apparatus or the like may be used, preferably, a centrifugal-flow, thin-film vacuum evaporator wherein, most preferably, the atmospheric pressure is reduced so as to allow evaporation of water at a temperature of about 40° C. It is the distillate of the green plant juice produced in this concentration step, a by-product normally disposed of as waste, that is utilized in the present invention. 
     In the course of the above-described procedures, various means, such as the replacement of air by an inert gas (e.g., nitrogen or argon), the inclusion of an oxygen absorber (e.g., glucose oxidase), maintenance at low temperatures and protection from light, may be used, alone or in any combination, to prevent the green plant juice from being discolored or deteriorated during transfer and storage preceding the drying step. 
     The distillate of the green plant juice produced in the concentration step may be utilized in the formulation of cosmetic compositions because of its strong antioxidant and antiseptic properties. 
     Cosmetic compositions are preparations applied to the surface of the body for the purpose of enhancing its appearance. These compositions can be make-up preparations, applied to bring about temporary effects, lasting only so long as the preparations remain on the body surface, or treatment preparations, which effect no immediately noticeable change but which, after repeated use, are expected to have a beautifying effect. 
     The present distillate of the green plant juice finds particular use in cosmetic compositions containing water, i.e. as a substitute for at least a portion of the pure water or distilled water normally compounded in such compositions. Generally, at least about 25% of the water should be replaced, in order to take advantage of the antioxidant and antiseptic properties of the distillate of the green plant juice, preferably at least about 50%, more preferably at least about 75%, and most preferably 100%. 
     The cosmetic compositions of the present invention may be skin care products such as lotions, creams, cleansers, etc. The compositions of the invention may be emulsions of liquid or semi-liquid consistency of the milk type, obtained by dispersion of an oil phase in an aqueous phase or vice versa; or suspensions or emulsions of soft consistency of the cream type. 
     All oils used in the production of cosmetic compositions are suited for use in the compositions of the present invention. There may be mentioned hydrocarbons such as mineral oils, petrolatum and squalane; animal and vegetable triglycerides such as almond oil, peanut oil, wheat germ oil, linseed oil, jojoba oil, oil of apricot pits, oil of walnuts, oil of palm nuts, oil of pistachio nuts, oil of sesame seeds, oil of rapeseed, cade oil, corn oil, peach pit oil, poppyseed oil, pine oil, castor oil, soybean oil, avocado oil, safflower oil, coconut oil, hazelnut oil, olive oil, grapeseed oil, and sunflower seed oil; hydroxy-substituted C 8 -C 50  unsaturated fatty acids and esters thereof; C 1 -C 24  esters of C 8 -C 30  saturated fatty acids such as isopropyl myristate, cetyl palmitate and octyldodecylmyristate (Wickenol 142); beeswax; saturated and unsaturated fatty alcohols such as behenyl alcohol and cetyl alcohol; fatty sorbitan esters; lanolin and lanolin derivatives; C 1 -C 24  esters of dimer and trimer acids such as diisopropyl dimerate, diisostearylmalate, diisostearyldimerate and triisostearyltrimerate; and silicones such as water-insoluble silicones inclusive of non-volatile polyalkyl and polyaryl siloxane gums and fluids, volatile cyclic and linear polyalkylsiloxanes, polyalkoxylated silicones, amino and quaternary ammonium modified silicones, rigid cross-linked and reinforced silicones and mixtures thereof. 
     While the distillate of the green plant juice of the present invention has antioxidant properties which may allow the preparation of compositions without the addition of other antioxidants, it is possible to use standard antioxidants such as t-butyl hydroquinone, butylated hydroxytoluene and α-tocopherol and its derivatives in the cosmetic compositions of the present invention, preferably, in amounts less than would normally be utilized. 
     Similarly, while the distillate of the green plant juice of the present invention has antiseptic properties, which may allow the preparation of compositions without the addition of other preservatives, it is possible to use standard preservatives such as methyl, ethyl, propyl, butyl and isobutyl p-hydroxybenzoate (parabems), 2-phenoxyethanol, sorbic acid, potassium sorbate, hexamidine diisothionate, imidazolidinylurea (Germall 115) or preservatives marketed under the names Kathon and Tridssan. 
     A wide variety of optional ingredients such as non-occlusive moisturizers, humectants, gelling agents, neutralizing agents, perfumes, coloring agents and surfactants can be added to the presently contemplated cosmetic compositions. 
     A humectant may be present in an amount of from about 0.1% to about 20%, preferably from about 1% to about 10% and especially from about 2% to about 5% by weight of the total composition. Suitable humectants include sorbitol, propylene glycol, butylene glycol, hexylene glycol, ethoxylated glucose derivatives, hexanetriol, glycerine, water-soluble polyglycerylmethacrylate lubricants (e.g., compositions available under the trademark Lubrajel) and panthenols (e.g. D-panthenol). 
     A hydrophilic gelling agent may be present in an amount of from about 0.01% to about 10%, preferably from about 0.02% to about 2% and especially from about 0.02% to about 0.5% by weight of the total composition. Suitable hydrophilic gelling agents include cellulose ethers (e.g., hydroxyethyl cellulose, hydroxypropylmethyl cellulose), polyvinylalcohol, guar gum, hydroxypropyl guar gum and xantham gum, as well as the acrylic acid/ethyl acrylate copolymers and the carboxyvinyl polymers sold under the trademark Carbopol. 
     Neutralizing agents, suitable for use in neutralizing acidic group containing hydrophilic gelling agents, include sodium hydroxide, potassium hydroxide, ammonium hydroxide, monoethanolamine, diethanolamine and triethanolamine. 
     Other optional materials include keratolytic agents such as salicylic acid; proteins and polypeptides and derivatives thereof; soluble or colloidally-soluble moisturizing agents such as hylaronic acid and starch-grafted sodium polyacrylates; coloring agents; perfumes and perfume solubilizers; surfactants/emulsifiers such as fatty alcohol ethoxylates and ethoxylated polyol fatty acid esters; and pigments which can be organic or inorganic and which include materials having a low color or lustre, such as matte finishing agents, and also light scattering agents. 
     The compositions of the present invention may be prepared by any conventional technique for preparing a cosmetic composition by merely substituting the distillate of green plant juice for the water normally incorporated into the composition. 
     The following examples are illustrative and are not intended to limit the invention in any way. 
     EXAMPLE 1 
     Young green leaves of barley (i.e., leaves and stems of barley before maturation) are thoroughly washed with water, disintegrated with a mixer, and squeezed. A green juice is obtained by filtering off fibrous residue. The green juice is vacuum distilled (pressure=about 55 mm Hg) in a centrifugal-flow-thin-film vacuum evaporator (EVAPOR®, Model No. CEP-305, made by Okawara Mfg. Co., Ltd. Shizuoka, Japan), the juice being poured on to the conical evaporating surface, rotating at 300 to 500 RPM, to form a thin film of about 0.1 mm thickness, with a residence time on the evaporating surface of only about one second. The outside of the rotating conical evaporating surface is jacketed and heated evenly by steam (inlet temp.=130° C., outlet temp.=80° C.). A tube at the edge of the rotating evaporating surface collects concentrate. 
     The distillate is a clear watery liquid with a very slightly greenish color and a refreshing grassy odor. 
     An analysis was conducted according to an internal standard method as described by L. S. Ettre in  The Practice of Gas Chromatography , Ettre, L. S., Zlatkis, A., Eds., Interscience Publishers: New York, 1967, p. 402. A Hewlett-Packard model HP5890 Series II gas chromatograph equipped with a 60 m×0.25 mm i.d. (d γ =1 μm) DB-WAX bonded-phase fused silica capillary column (J&amp;W Scientific, Folsom, Calif.) was used and interfaced to an HP5791A mass selective detector for mass spectral identification of the components. The linear velocity of the helium carrier gas was 30 cm/sec, the oven temperature was programmed from 50° C. to 200° C. at 3° C./min and held for 40 minutes, and the ionization voltage for mass spectral identification was 70 eV. 
     An analysis is shown in Table A. 
     
       
         
               
               
               
               
             
               
               
               
               
               
             
           
               
                 TABLE A 
               
               
                   
               
               
                 No. 
                 R. TIME 
                 R. Index 
                 CONC COMPOUNDS 
               
               
                   
               
             
             
               
                   
               
             
          
           
               
                 1 
                 2.762 
                 0 
                 0.01 
                   
               
               
                 2 
                 2.860 
                 0 
                 0.00 
                 3-methyl-1-butene 
               
               
                 3 
                 2.908 
                 0 
                 0.00 
                   
               
               
                 4 
                 2.962 
                 0 
                 0.01 
                   
               
               
                 5 
                 3.060 
                 600 
                 0.00 
                   
               
               
                 6 
                 3.317 
                 702 
                 0.01 
                 acetaldehyde 
               
               
                 7 
                 3.950 
                 792 
                 0.18 
                 propanal 
               
               
                 8 
                 4.291 
                 820 
                 0.01 
                   
               
               
                 9 
                 4.486 
                 833 
                 0.01 
                   
               
               
                 10 
                 4.603 
                 841 
                 0.00 
                   
               
               
                 11 
                 5.458 
                 900 
                 0.02 
                   
               
               
                 12 
                 5.560 
                 904 
                 0.02 
                 butanal 
               
               
                 13 
                 6.362 
                 933 
                 0.01 
                   
               
               
                 14 
                 6.511 
                 939 
                 0.00 
                   
               
               
                 15 
                 6.701 
                 945 
                 0.08 
                 2-ethylfuran 
               
               
                 16 
                 7.022 
                 957 
                 0.00 
                   
               
               
                 17 
                 7.428 
                 972 
                 0.54 
                 3-pentanone 
               
               
                 18 
                 7.548 
                 977 
                 0.01 
                   
               
               
                 19 
                 7.638 
                 980 
                 0.01 
                   
               
               
                 20 
                 7.824 
                 987 
                 0.02 
                 2-methyl-3-buten-2-one 
               
               
                 21 
                 8.101 
                 997 
                 0.02 
                   
               
               
                 22 
                 8.557 
                 1009 
                 0.01 
                 2-methyl-2-butanol 
               
               
                 23 
                 8.992 
                 1019 
                 7.42 
                 1-penten-3-one 
               
               
                 24 
                 9.280 
                 1025 
                 0.00 
                   
               
               
                 25 
                 9.430 
                 1029 
                 0.00 
                   
               
               
                 26 
                 9.573 
                 1032 
                 0.02 
                 (E)-2-butenal 
               
               
                 27 
                 9.780 
                 1037 
                 0.00 
                   
               
               
                 28 
                 9.850 
                 1039 
                 0.00 
                   
               
               
                 29 
                 10.023 
                 1043 
                 0.00 
                   
               
               
                 30 
                 10.423 
                 1052 
                 0.03 
                 2,3-pentanedione 
               
               
                 31 
                 10.751 
                 1059 
                 0.00 
                   
               
               
                 32 
                 11.279 
                 1072 
                 0.01 
                   
               
               
                 33 
                 11.465 
                 1076 
                 0.42 
                 hexanal 
               
               
                 34 
                 11.749 
                 1083 
                 0.01 
                   
               
               
                 35 
                 12.594 
                 1102 
                 0.02 
                   
               
               
                 36 
                 12.850 
                 1106 
                 0.00 
                   
               
               
                 37 
                 13.013 
                 1109 
                 0.04 
                 3-pentanol 
               
               
                 38 
                   
                   
                 t 
                 2-pentanol 
               
               
                 39 
                 13.769 
                 1123 
                 `0.82 
                 (E)-2-pentenal 
               
               
                 40 
                 14.287 
                 1132 
                 0.10 
                 (E)-3-hexenal 
               
               
                 41 
                 14.585 
                 1137 
                 0.22 
                 (Z)-3-hexenal 
               
               
                 42 
                 16.226 
                 1166 
                 22.12 
                 1-penten-3-ol 
               
               
                 43 
                 16.540 
                 1172 
                 0.00 
                   
               
               
                 44 
                 16.939 
                 1179 
                 0.02 
                 3-penten-2-ol 
               
               
                 45 
                 17.565 
                 1190 
                 0.01 
                   
               
               
                 46 
                 17.930 
                 1196 
                 0.21 
                 (Z)-2-hexenal 
               
               
                 47 
                 19.341 
                 1219 
                 14.55 
                 (E)-2-hexenal 
               
               
                 48 
                 20.369 
                 1235 
                 0.05 
                   
               
               
                 49 
                 21.431 
                 1252 
                 0.17 
                 pentanol 
               
               
                 50 
                 22.560 
                 1269 
                 0.01 
                   
               
               
                 51 
                 23.141 
                 1279 
                 0.08 
                 3-hydroxybutan-2-one 
               
               
                 52 
                 23.720 
                 1288 
                 0.01 
                   
               
               
                 53 
                 24.040 
                 1293 
                 0.00 
                   
               
               
                 54 
                 24.280 
                 1296 
                 0.00 
                   
               
               
                 55 
                 25.430 
                 1314 
                 0.42 
                 (E)-2-pentenol 
               
               
                 56 
                 26.564 
                 1332 
                 34.67 
                 (Z)-2-pentenol 
               
               
                 57 
                 27.160 
                 1341 
                 0.07 
                   
               
               
                 58 
                 27.480 
                 1346 
                 0.05 
                   
               
               
                 59 
                 28.176 
                 1356 
                 0.37 
                 hexanol 
               
               
                 60 
                 28.176 
                 1356 
                 0.05 
                 2-hydroxypentan-3-one 
               
               
                 61 
                 28.757 
                 1365 
                 0.15 
                 (E)-3-hexenol 
               
               
                 62 
                   
                   
                   
                   
               
               
                 63 
                 30.263 
                 1388 
                 4.27 
                 (Z)-3-hexanol 
               
               
                 64 
                 30.708 
                 1395 
                 0.14 
                 (E,E)-2,4-hexadienal 
               
               
                 65 
                 31.200 
                 1403 
                 0.02 
                   
               
               
                 66 
                 31.578 
                 1408 
                 0.82 
                 (E)-2-hexanol 
               
               
                 67 
                 32.330 
                 1420 
                 0.03 
                 (E)-2-octenal 
               
               
                 68 
                 34.345 
                 1451 
                 0.03 
                 1-octen-3-ol 
               
               
                 69 
                 34.776 
                 1458 
                 0.21 
                 (E,Z)-2,4-heptadienal 
               
               
                 70 
                 36.537 
                 1485 
                 0.11 
                 (E,E)-2,4-heptadienal 
               
               
                 71 
                 36.537 
                 1485 
                 0.01 
                 (Z)-1,5-octadlen-3-ol 
               
               
                 72 
                 36.920 
                 1491 
                 0.01 
                 2-ethylhexanol 
               
               
                 73 
                 38.418 
                 1515 
                 0.18 
                   
               
               
                 74 
                 38.920 
                 1523 
                 0.17 
                   
               
               
                 75 
                   
                   
                 t 
                 propanoic acid 
               
               
                 76 
                 39.669 
                 1535 
                 0.12 
                 4-oxohexanal 
               
               
                 77 
                 40.000 
                 1540 
                 0.06 
                   
               
               
                 78 
                 41.251 
                 1560 
                 0.56 
                 octanol 
               
               
                 79 
                 42.080 
                 1574 
                 0.02 
                   
               
               
                 80 
                 42.386 
                 1579 
                 0.04 
                 (E,Z)-2,6-nonadienal 
               
               
                 81 
                 42.897 
                 1587 
                 0.19 
                   
               
               
                 82 
                 43.389 
                 1595 
                 0.12 
                 2-hydroxy-2,6,6- 
               
               
                   
                   
                   
                   
                 trimethylcyclohexanone 
               
               
                 83 
                 43.800 
                 1601 
                 0.02 
                   
               
               
                 84 
                 44.215 
                 1608 
                 0.39 
                   
               
               
                 85 
                 44.720 
                 1617 
                 0.09 
                 beta-cyclocitral 
               
               
                 86 
                 45.445 
                 1629 
                 0.12 
                   
               
               
                 87 
                 46.160 
                 1641 
                 0.03 
                 3-hydroxyoctan-2-one 
               
               
                 88 
                 46.649 
                 1649 
                 0.28 
                   
               
               
                 89 
                 47.640 
                 1666 
                 0.00 
                   
               
               
                 90 
                 48.123 
                 1674 
                 0.07 
                 5-methyl-2(5H)-furanone 
               
               
                 91 
                 49.006 
                 1689 
                 1.62 
                   
               
               
                 92 
                 49.923 
                 1704 
                 0.43 
                   
               
               
                 93 
                 51.000 
                 1723 
                 0.00 
                   
               
               
                 94 
                 51.440 
                 1731 
                 0.02 
                   
               
               
                 95 
                 51.920 
                 1739 
                 0.01 
                   
               
               
                 96 
                 52.533 
                 1750 
                 0.38 
                 5-ethyl-2(5H)- 
               
               
                   
                   
                   
                   
                 furanone (T) 
               
               
                 97 
                 52.799 
                 1755 
                 0.14 
                   
               
               
                 98 
                 53.314 
                 1764 
                 0.24 
                   
               
               
                 99 
                 54.303 
                 1781 
                 0.04 
                   
               
               
                 100 
                 54.678 
                 1788 
                 0.14 
                   
               
               
                 101 
                 55.197 
                 1797 
                 0.03 
                   
               
               
                 102 
                 55.921 
                 1810 
                 0.10 
                   
               
               
                 103 
                 56.440 
                 1819 
                 0.06 
                   
               
               
                 104 
                 57.130 
                 1832 
                 0.13 
                   
               
               
                 105 
                 57.517 
                 1839 
                 0.10 
                   
               
               
                 106 
                 58.040 
                 1849 
                 0.03 
                 hexanoic acid 
               
               
                 107 
                 58.640 
                 1860 
                 0.00 
                   
               
               
                 108 
                 58.910 
                 1864 
                 0.04 
                   
               
               
                 109 
                 59.375 
                 1873 
                 0.05 
                   
               
               
                 110 
                 59.375 
                 1873 
                 0.11 
                   
               
               
                 111 
                 59.960 
                 1884 
                 0.01 
                 (E,E,E)-2,4,6-nonatrienal 
               
               
                 112 
                 60.400 
                 1892 
                 0.02 
                   
               
               
                 113 
                 60.734 
                 1898 
                 0.02 
                   
               
               
                 114 
                 61.250 
                 1908 
                 0.09 
                 phenylethyl alcohol 
               
               
                 115 
                 61.720 
                 1917 
                 0.06 
                   
               
               
                 116 
                 62.414 
                 1930 
                 0.26 
                   
               
               
                 117 
                 62.829 
                 1938 
                 0.15 
                 beta-ionone 
               
               
                 118 
                 63.429 
                 1949 
                 0.07 
                   
               
               
                 119 
                 63.884 
                 1958 
                 0.08 
                   
               
               
                 120 
                 64.246 
                 1965 
                 0.61 
                   
               
               
                 121 
                 64.906 
                 1978 
                 0.40 
                   
               
               
                 122 
                 65.312 
                 1985 
                 0.15 
                 5,6-epoxy-beta-ionone 
               
               
                 123 
                 65.920 
                 1997 
                 0.24 
                   
               
               
                 124 
                 66.895 
                 2016 
                 0.07 
                   
               
               
                 125 
                 67.461 
                 2028 
                 0.17 
                   
               
               
                 126 
                 68.800 
                 2055 
                 0.02 
                   
               
               
                 127 
                 69.135 
                 2061 
                 0.04 
                   
               
               
                 128 
                 69.480 
                 2068 
                 0.01 
                   
               
               
                 129 
                 70.035 
                 2079 
                 0.03 
                   
               
               
                 130 
                 70.413 
                 2087 
                 0.06 
                   
               
               
                 131 
                 70.966 
                 2098 
                 0.04 
                 2,6-di-tert-butyl-4- 
               
               
                   
                   
                   
                   
                 hydroxy-4-methyl-2,5- 
               
               
                   
                   
                   
                   
                 cyclohexadlen-1-one (T) 
               
               
                 132 
                 71.600 
                 2111 
                 0.29 
                   
               
               
                 133 
                 72.179 
                 2123 
                 0.07 
                   
               
               
                 134 
                 72.763 
                 2135 
                 0.05 
                   
               
               
                 135 
                 73.245 
                 2145 
                 0.04 
                   
               
               
                 136 
                 74.000 
                 2161 
                 0.03 
                   
               
               
                 137 
                 74.400 
                 2169 
                 0.02 
                   
               
               
                 138 
                 75.257 
                 2187 
                 0.40 
                   
               
               
                 139 
                 75.610 
                 2195 
                 0.14 
                   
               
               
                 140 
                 76.782 
                 2220 
                 0.09 
                   
               
               
                 141 
                 77.497 
                 2235 
                 0.01 
                   
               
               
                 142 
                 77.920 
                 2244 
                 0.01 
                   
               
               
                 143 
                 78.342 
                 2254 
                 0.04 
                   
               
               
                 144 
                 78.778 
                 2263 
                 0.03 
                   
               
               
                 145 
                 79.347 
                 2275 
                 0.02 
                   
               
               
                 146 
                 79.680 
                 2283 
                 0.01 
                   
               
               
                 147 
                 80.026 
                 2290 
                 0.02 
                   
               
               
                 148 
                 81.920 
                 2331 
                 0.03 
                 dihydroactinidiolide 
               
               
                 149 
                 81.920 
                 2331 
                 0.03 
                   
               
               
                 150 
                 82.664 
                 2347 
                 0.04 
                   
               
               
                 151 
                 83.417 
                 2363 
                 0.01 
                 diethyl phthalate 
               
               
                 152 
                 84.629 
                 2389 
                 0.02 
                   
               
               
                 153 
                 85.118 
                 2400 
                 0.04 
                 tetracosane 
               
               
                 154 
                 85.587 
                 2408 
                 0.07 
                   
               
               
                 155 
                 86.787 
                 2429 
                 0.03 
                   
               
               
                 156 
                 87.360 
                 2439 
                 0.01 
                   
               
               
                 157 
                 87.677 
                 2445 
                 0.05 
                   
               
               
                 158 
                 88.980 
                 2468 
                 0.02 
                   
               
               
                 159 
                 90.141 
                 2489 
                 0.05 
                   
               
               
                 160 
                 91.346 
                 2508 
                 0.02 
                 pentacosane 
               
               
                 161 
                 92.293 
                 2521 
                 0.03 
                 phytyl acetate 
               
               
                 162 
                 93.018 
                 2531 
                 0.02 
                 diisobutyl phthalate 
               
               
                 163 
                 93.491 
                 2538 
                 0.01 
                   
               
               
                 164 
                 93.791 
                 2542 
                 0.01 
                   
               
               
                 165 
                 94.411 
                 2551 
                 0.01 
                 vanillin 
               
               
                 166 
                 94.960 
                 2559 
                 0.01 
                   
               
               
                 167 
                 95.497 
                 2566 
                 0.01 
                   
               
               
                 168 
                 95.987 
                 2573 
                 0.01 
                   
               
               
                 169 
                 96.586 
                 2581 
                 0.01 
                   
               
               
                 170 
                 97.234 
                 2590 
                 0.10 
                 octadecanol 
               
               
                 171 
                 97.880 
                 2599 
                 0.01 
                 hexacosane 
               
               
                 172 
                 98.820 
                 2610 
                 0.07 
                 phytol 
               
               
                 173 
                 100.251 
                 2625 
                 0.01 
                 4-hydroxy-3- 
               
               
                   
                   
                   
                   
                 methoxyacetophenone 
               
               
                 174 
                 101.071 
                 2634 
                 0.03 
                   
               
               
                 175 
                 102.299 
                 2647 
                 0.05 
                   
               
               
                 176 
                 103.240 
                 2657 
                 0.01 
                   
               
               
                 177 
                 105.148 
                 2677 
                 0.01 
                   
               
               
                 178 
                 105.790 
                 2684 
                 0.04 
                   
               
               
                 179 
                 106.463 
                 2691 
                 0.15 
                 dibutyl phthalate 
               
               
                 180 
                 107.278 
                 2700 
                 0.01 
                 heptacosane 
               
               
                 181 
                 109.078 
                 2714 
                 0.01 
                   
               
               
                 182 
                 114.139 
                 2755 
                 0.02 
                   
               
               
                 183 
                 118.800 
                 2793 
                 0.17 
                 bis(2-ethylhexyl) adipate 
               
               
                   
               
             
          
         
       
     
     EXAMPLE 2 
     250 ml of the distillate produced by the technique of Example 1 is extracted with 50 ml of dichloromethane using a liquid-liquid continuous extractor for 6 hours. The solvent is separated from the extract by using a rotary evaporator and further condensation is achieved under a purified nitrogen stream. 
     The extract is examined for antioxidative activity using an aldehyde/acid oxidation system. The method used is based on the auto-oxidation of aldehydes to carboxylic acids with active oxygen species such as hydroxy radical as discussed in  Autoxidation of various organic substances , Horner, L.,  Autoxidation and Antioxidants , Lundberg, W. O., Ed., John Wiley &amp; Sons, New York, 1961, pp. 197-202. The results, illustrated in FIG. 1, show that the extract inhibited oxidation of hexanol more than two weeks at the level of 50 ppm. This activity is almost equal to that of the well-known antioxidant, α-tocopherol. 
     A gas chromatogram of the extract shows more than 100 peaks, suggesting that the distillate contains many volatile chemicals some of which possess a potent antioxidant activity. 
     EXAMPLE 3 
     The distillate produced by the technique of Example 1 is passed through a 0.45 μm membrane filter to remove any barley juice residues. 
     Apples are peeled and immersed in regular tap water, filtered distillate or tap water containing salt for five minutes. The apples are then taken out and allowed to sit for 1 hour, whereupon their color is determined. The results are set forth in Table 1. 
     
       
         
               
               
             
           
               
                 TABLE 1 
               
               
                   
               
               
                 IMMERSION LIQUID 
                 COLOR 
               
               
                   
               
             
             
               
                 Tap Water  
                 80% of the surface becomes 
               
               
                   
                 brown or tan 
               
               
                 Filtered Distillate 
                 less than 5% of the surface 
               
               
                   
                 becomes brown 
               
               
                 Tap Water Containing Salt 
                 less than 5% of the surface 
               
               
                   
                 becomes brown 
               
               
                   
               
             
          
         
       
     
     EXAMPLE 4 
     Cut tulips are kept in tap water or the filtered distillate as in Example 3. The water and the filtered distillate are changed every other day. The result is shown in Table 2. 
     
       
         
               
               
             
               
               
             
           
               
                 TABLE 2 
               
             
             
               
                   
               
               
                   
                 Number of Days That 
               
               
                 Liquid 
                 Tulips Lasted 
               
               
                   
               
             
          
           
               
                 Tap Water  
                 5 
               
               
                 Filtered  Distillate 
                 10 
               
               
                   
               
             
          
         
       
     
     The tulips in filtered distillate last longer and are in better condition than those in tap water. 
     EXAMPLE 5 
     Two facial toners are prepared as set forth in Table 3. 
     
       
         
               
               
             
               
               
               
             
               
               
               
               
               
             
               
               
               
             
               
               
               
               
               
             
           
               
                   
                 TABLE 3 
               
             
             
               
                   
                   
               
               
                   
                 TONER 
               
             
          
           
               
                 INGREDIENT 
                 A  (1)   
                 B 
               
               
                   
               
             
          
           
               
                 Butylene glycol 
                 60 
                 g 
                 60 
                 g 
               
               
                 Sorbitol 
                 20 
                 g 
                 20 
                 g 
               
               
                 Glycerin 
                 20 
                 g 
                 20 
                 g 
               
               
                 Methylparaben 
                 0.6 
                 g 
                 0.3 
                 g 
               
               
                 Phenoxyethanol 
                 0.5 
                 g 
                 0.5 
                 g 
               
               
                 Sodium citrate 
                 0.1 
                 g 
                 0.1 
                 g 
               
               
                 Butylparaben 
                 0.1 
                 g 
                 0.05 
                 g 
               
               
                 Propylparaben 
                 0.1 
                 g 
                 0.05 
                 g 
               
               
                 Citric acid 
                 0.02 
                 g 
                 0.02 
                 g 
               
             
          
           
               
                 Distilled H 2 O 
                 balance 
                 — 
               
               
                 Filtered  Distillate (Ex. 3) 
                 — 
                 balance 
               
             
          
           
               
                 Total 
                 1,000 
                 g 
                 1,000 
                 g 
               
               
                   
               
               
                   (1)  - commercial product in Japan  
               
             
          
         
       
     
     18 ml. of toner A, 18 ml of toner B and 18 ml of a toner having the same formulation as toner A except for being devoid of preservatives are each inoculated with 2 ml of Staphylococcus aureus solution (Staphylococcus aureus in sterile diluent (pepton, lecithin, distilled water) at a concentration between 1×10 6  and 1×10 7 ) to make sample solutions A, B and C, respectively. Sample A, B and C are allowed to stand at room temperature and sampled at day 0, day 1, day 3, day 7, day 14 and day 21. Each time 1 ml of solution is taken and general bacteria plate count tests are performed. In the plate count tests, 1 ml. of sample solution and 20 ml of media are placed in a Petri dish, cultivated at 36° C. for 48 hours, and the number of colonies reported. Serial dilutions, such as {fraction (1/10)}, {fraction (1/100)}, {fraction (1/1000)}, etc., are done if the colonies number more than 200 and the test procedures are repeated. The results are set forth in Table 4. 
     
       
         
               
               
             
               
               
               
               
             
               
               
               
               
             
           
               
                   
                 TABLE 4 
               
             
             
               
                   
                   
               
               
                   
                 SAMPLE 
               
             
          
           
               
                   
                 A 
                 B 
                 C 
               
               
                   
                   
               
             
          
           
               
                 Day 0 
                 2.7 × 10 5   
                 1.5 × 10 5   
                 1.5 × 10 5   
               
               
                 Day 1 
                 6.8 
                 5.5 
                 2.5 × 10 4   
               
               
                 Day 3 
                 0 
                 0.5 
                 5.9 × 10 7   
               
               
                 Day 7 
                 0 
                 0 
                 3.3 × 10 7   
               
               
                 Day 14 
                 0 
                 0 
                 4.9 × 10 7   
               
               
                 Day 21 
                 0 
                 0 
                 2.4 × 10 7   
               
               
                   
               
             
          
         
       
     
     Samples A and B have similar antibacterial activities. Therefore, filtered distillate may be used in a cosmetic product to reduce the required amount of preservatives. 
     EXAMPLE 6 
     A toner having the following composition is prepared using the filtered distillate as in Example 3. 
     
       
         
               
               
               
               
             
               
               
               
             
               
               
               
               
             
           
               
                   
                   
               
             
             
               
                   
                 95% Ethanol 
                 100 
                 g 
               
               
                   
                 Methyl p-hydroxybenzoate 
                 0.05 
                 g 
               
               
                   
                 Perfume 
                 0.5 
                 g 
               
               
                   
                 Colorant 
                 0.005 
                 g 
               
             
          
           
               
                   
                 Filtered  distillate 
                 Balance 
               
             
          
           
               
                   
                   
                 1,000 
                 g 
               
               
                   
                   
               
             
          
         
       
     
     This toner is used everyday after washing the face in the morning and before sleeping to examine the effect on spots and freckles. Evaluation was effected by comparing spots and freckles before and after a 6-week application period. The results obtained on a panel of 20 women are shown in Table 5. 
     
       
         
               
               
               
             
           
               
                 TABLE 5 
               
               
                   
               
               
                 EFFECT 
                 COLOR (1)   
                 BOUNDARY (2)   
               
               
                   
               
             
             
               
                 Effective 
                 5 
                 7 
               
               
                 Slightly effective 
                 7 
                 8 
               
               
                 No effect 
                 8 
                 5 
               
               
                   
               
               
                   (1)  - Color of spots and freckles  
               
               
                 Dark Brown  No effect  
               
               
                 Pale Brown  Slightly effective  
               
               
                 Almost none  Effective  
               
             
          
         
       
     
     (2)—Boundary Between Snot or Freckle and Other Regular Skin Areas 
     Boundary apparent No effect 
     Boundary unclear Slightly effective 
     Boundary almost undiscernible Effective