JP6286602B2 - Blackening accelerator for skin and hair, external preparation for promoting blackening, and food and drink for promoting blackening containing the blackening accelerator - Google Patents
Blackening accelerator for skin and hair, external preparation for promoting blackening, and food and drink for promoting blackening containing the blackening accelerator Download PDFInfo
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- JP6286602B2 JP6286602B2 JP2017115651A JP2017115651A JP6286602B2 JP 6286602 B2 JP6286602 B2 JP 6286602B2 JP 2017115651 A JP2017115651 A JP 2017115651A JP 2017115651 A JP2017115651 A JP 2017115651A JP 6286602 B2 JP6286602 B2 JP 6286602B2
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- blackening
- skin
- hair
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Description
本発明は、皮膚や毛髪の黒化を促進する黒化促進剤と、その黒化促進剤を含む外用剤または飲食品に関する。詳しくは、ヒュウガトウキ(学名Angelica furcijuga Kitagawa、以下、単に「ヒュウガトウキ」という。)を有効成分とする、皮膚または毛髪の黒化促進剤、外用剤、飲食品の発明に関する。 The present invention relates to a blackening accelerator that promotes blackening of skin and hair, and an external preparation or food or drink containing the blackening accelerator. More specifically, the present invention relates to a skin or hair blackening promoter, an external preparation, and an invention for foods and drinks containing Hyugatoki (scientific name Angelica furcijuga Kitagawa, hereinafter simply referred to as “Hyugatoki”) as an active ingredient.
ヒュウガトウキは、セリ科植物のシシウド属に属し、九州南部の丘陵や山地に生える多年性植物である。
近年ではその効能の理活性が注目され、例えば、食欲増進、疲労回復、代謝機能の正常化に用いること(特許文献1など参照)、抗肝炎剤、抗がん剤として用いること(特許文献2、特許文献3など参照)などが提案されている。
Hyugatouki is a perennial plant that belongs to the genus Shisiudo, a celery family, and grows in the hills and mountains of southern Kyushu.
In recent years, the physical activity of its efficacy has attracted attention. For example, it is used for appetite enhancement, fatigue recovery, normalization of metabolic function (see Patent Document 1 etc.), antihepatitis agent, anticancer agent (Patent Document 2). , Patent Document 3, etc.) have been proposed.
また最近では、トウキ類からの抽出物による美白効果、すなわち、メラニンの生成を抑制する作用にも注目が集まっている。
毛髪や皮膚の色を決定するメラニン色素は、メラノサイト(メラニン合成細胞)内のメラノソームでチロシンから生合成される。紫外線や乾燥などの外的要因、老化やストレスなどの内的要因の影響によりメラニン色素が増加すると、皮膚の色に冴えが無く艶や透明感が損なわれる「肌のくすみ」が誘発される。多くの女性が美容上の悩みとして肌のくすみを挙げている。
このような問題を改善するために、例えば、特許文献4、特許文献5、特許文献6などには、トウキ類からの抽出物がメラニンの生成を抑制し、美白剤として有用であることが開示されている。
Recently, attention has also been focused on the whitening effect by the extract from Toki, that is, the action of suppressing the production of melanin.
Melanin pigments that determine the color of hair and skin are biosynthesized from tyrosine at melanosomes in melanocytes (melanin synthesizing cells). When the melanin pigment increases due to the influence of external factors such as ultraviolet rays and dryness, and internal factors such as aging and stress, it causes “skin dullness” that does not make the skin color dull and loses its gloss and transparency. Many women list dull skin as a cosmetic problem.
In order to improve such problems, for example, Patent Literature 4, Patent Literature 5, Patent Literature 6 and the like disclose that an extract from Tokis suppresses the production of melanin and is useful as a whitening agent. Has been.
一方、メラノサイトのメラニンの産生量が少なくなると、白髪の直接的な原因になると共に、肌を黒くしたい者にとっては、思いどおりに皮膚を黒くすることが困難になる。
白髪は老化やストレス等により、メラノサイトやメラノソームの減少、またはこれら細胞や器官の異常によるチロシナーゼの量や活性の低下、メラノソームの輸送阻害等が関与すると考えられている。
日本人の場合、黒色又は茶褐色などの髪が一般に好まれるが、加齢の結果として白髪が多く現れる。これは、毛根部などに存在するメラニン細胞の数や活性の低下によりメラニンが著しく減少することによるもので、美容的および心理的にも敬遠される傾向にある。
On the other hand, when the amount of melanin produced by melanocytes decreases, it becomes a direct cause of gray hair, and it becomes difficult for those who want to darken the skin to make it black as expected.
It is considered that gray hair is associated with a decrease in melanocytes and melanosomes due to aging and stress, or a decrease in the amount and activity of tyrosinase due to abnormalities in these cells and organs, and inhibition of melanosome transport.
In the case of Japanese, black or brownish hair is generally preferred, but many gray hairs appear as a result of aging. This is due to a marked decrease in melanin due to a decrease in the number and activity of melanocytes present in the hair roots, etc., and there is a tendency to be shunned cosmetically and psychologically.
抗白髪剤については、白髪の発生機序やメラニン色素形成機序等を参考に、有効物質をスクリーニングするか、または、無作為に各種物質の白髪防止作用を検討することによって得られた多種多様な成分の使用が提案されている。
例えば、特許文献7にはイチジクやクワなどの抽出物が、特許文献8にはアキノノゲシの抽出物が、皮膚や毛髪の黒化に有用であることが開示されている。
With regard to anti-whitening agents, there are a wide variety of products obtained by screening for effective substances with reference to the mechanism of white hair development and the mechanism of melanin pigment formation, or by examining the white hair prevention action of various substances at random. The use of various ingredients has been proposed.
For example, Patent Document 7 discloses that extracts such as figs and mulberries are useful for darkening skin and hair, and Patent Document 8 discloses extracts of Akinonogeshi.
また、人の皮膚は紫外線に長期間曝露されると、紅斑、浮腫、蕁麻疹、肝斑(シミ)、雀卵斑(ソバカス)や皮膚の老化(皮膚萎縮、しわ、乾皮症状、皮膚異常角化など)、老人性色素斑、黒皮症、更に皮膚癌の危険など短期的および長期的に健康に悪影響が及ぶすことが知られている。白人などは日光性皮膚癌にかかりやすく、黒色腫(皮膚癌)のリスクが高い。有色人種でも日光に長期曝露されると、皮膚癌や皮膚老化促進のリスクが増大する。
他方、皮膚においてメラニンは紫外線の有害な作用から皮膚を守る働きをしており、紫外線照射時に生成され、肌の褐色化等に大きく影響している。
In addition, when human skin is exposed to ultraviolet rays for a long time, erythema, edema, urticaria, liver spots (spots), sparrow eggs (sobacas) and skin aging (skin atrophy, wrinkles, dry skin symptoms, skin abnormalities) Such as keratinization), senile pigment spots, melanosis, and the risk of skin cancer are known to adversely affect health in the short and long term. Caucasians and others are prone to sunlight skin cancer and are at increased risk of melanoma (skin cancer). Long-term exposure to sunlight, even for colored people, increases the risk of skin cancer and accelerated skin aging.
On the other hand, in the skin, melanin has a function of protecting the skin from the harmful effects of ultraviolet rays, and is produced when irradiated with ultraviolet rays, and greatly affects the browning of the skin.
最近の若年層は日焼けした肌色を好む傾向も一部では見られる。このような若者の多くは、限られた範囲(サンタン領域)の自然光、または、特別に設計された紫外線光源を照射して人工的にメラニンを産生する手段を利用している。しかし、この行為は前記したように皮膚の健康に悪影響が及ぶおそれがあり、前記したような天然植物由来の皮膚の黒化剤が求められている。 Some young people tend to like tanned skin tones. Many of these young people use a means of artificially producing melanin by irradiating a limited range (suntan region) of natural light or a specially designed ultraviolet light source. However, this action may adversely affect the health of the skin as described above, and there is a need for a natural plant-derived skin blackening agent as described above.
以上説明したように、本発明者らが知る限りにおいて、ヒュウガトウキが毛髪および皮膚の黒化促進に有用であることは見出されていない。 As described above, as far as the present inventors know, it has not been found that Hyugatouki is useful for promoting the darkening of hair and skin.
本発明はこのような従来事情に鑑みてなされたもので、その目的とするところは、実使用における安全性を確保すると共に、優れた皮膚および毛髪の黒化促進剤効果を示す、新規な皮膚または毛髪の黒化促進剤、外用剤、飲食品を提供することである。 The present invention has been made in view of such conventional circumstances, and the object of the present invention is to provide a novel skin that ensures safety in actual use and exhibits excellent skin and hair blackening accelerator effects. Or it is providing the blackening promoter of hair, an external preparation, and food-drinks.
上記課題を解決するために本発明者らは鋭意検討を重ねた結果、ヒュウガトウキの抽出物に、優れた皮膚および毛髪の黒化促進効果があることを初めて見出し、本発明を完成するに至った。 In order to solve the above-mentioned problems, the present inventors have conducted intensive studies, and as a result, for the first time, the extract of Hyugatouki has an excellent skin and hair blackening promoting effect, and the present invention has been completed. It was.
すなわち、本発明は、ヒュウガトウキの葉部および茎部の抽出物を単独の有効成分としたメラニン色素の増加促進剤を含む皮膚および/または毛髪の黒化促進用健康食品または健康飲料である。 That is, the present invention is a health food or health drink for promoting skin and / or hair blackening, which contains an increase promoter for melanin pigment comprising a leaf and stem extract of Hyugatouki as a single active ingredient .
また、本発明は、ヒュウガトウキの葉部および茎部の抽出物を単独の有効成分としたメラニン色素の増加促進剤を含む皮膚および/または毛髪の黒化促進用保健機能食品または保健機能飲料である。 The present invention also relates to a health functional food or health functional drink for promoting skin and / or hair blackening comprising a melanin increase promoter comprising a leaf and stem extract of Hyugatouki as a single active ingredient. is there.
また、本発明は、ヒュウガトウキの葉部および茎部の抽出物を単独の有効成分としたメラニン色素の増加促進剤を含む皮膚および/または毛髪の黒化促進用栄養補助食品である。The present invention is also a nutritional supplement for promoting skin and / or hair blackening, comprising a melanin increase promoter comprising a leaf and stem extract of Hyugatouki as a single active ingredient.
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以上説明したように本発明は、天然由来の植物であるヒュウガトウキの抽出物を有効成分とした新規な皮膚および毛髪の黒化促進剤、外用剤、飲食品であって、実使用に対する安全性を有すると共に、皮膚および毛髪の黒化促進に対し優れた効果を示す。 As described above, the present invention is a novel skin and hair blackening promoter, external preparation, food and drink comprising an extract of Hyugatouki, which is a naturally derived plant, as an active ingredient, and is safe for practical use. And has an excellent effect on promoting the blackening of skin and hair.
以下、本発明についてさらに詳述する。
(黒化促進剤)
本発明では前述したように、ヒュウガトウキの抽出物を有効成分として用いる。
ヒュウガトウキの抽出物を得るにあたり、葉部、茎部、花部等の地上部、種子、根部、あるいは全草をそのままなど、適宜任意に用いることが考えられるが、葉部、茎部等の地上部を用いることがより好ましい。またヒュウガトウキは、生のままのもの、または乾燥したもの、いずれも用いることができ、必要に応じて切断又は粉砕などし、適宜な抽出溶媒にて抽出操作が行われる。
Hereinafter, the present invention will be described in further detail.
(Blackening accelerator)
In the present invention, as described above, the extract of Hyugatouki is used as an active ingredient.
In obtaining the extract of Hyugatouki, it is conceivable to arbitrarily use the ground part such as the leaf part, the stem part, the flower part, the seed, the root part, or the whole plant as it is, but the leaf part, the stem part, etc. It is more preferable to use the above-ground part. Moreover, the raw ginger can be either raw or dried, and is cut or pulverized as necessary, and an extraction operation is performed with an appropriate extraction solvent.
抽出溶媒としては、極性溶媒、非極性溶媒、またはこれらの混合物など、植物抽出に通常用いられる溶媒であればいずれも用いることができる。 As the extraction solvent, any solvent that is usually used for plant extraction, such as a polar solvent, a nonpolar solvent, or a mixture thereof, can be used.
具体的には、極性溶媒として、水または熱水、アルコール類(メタノール、エタノール、イソプロパノール、n−プロパノール、イソブタノール、n−ヘキサノール、メチルアミルアルコール2−エチルブタノール、n−オクタノール等)、多価アルコールまたはその誘導体類(エチレングリコール、エチレングリコールモノメチルエーテル、エチレングリコールモノエチルエーテル、プロピレングリコール、プロピレングリコールモノメチルエーテル、プロピレングリコールモノエチルエーテル、トリエチレングリコール、1,3−ブチレングリコール、ヘキシレングリコール等)、ケトン類(アセトン、メチルアセトン、メチルエチルケトン、メチルイソブチルケトン、メチル−n−プロピルケトン等)、エステル類(酢酸エチル、酢酸イソプロピル等)、エーテル類(エチルエーテル、イソプロピルエーテル、n−ブチルエーテル等)、などのうちの一種、またはこれら二種以上の混合溶媒を挙げることができる。 Specifically, as a polar solvent, water or hot water, alcohols (methanol, ethanol, isopropanol, n-propanol, isobutanol, n-hexanol, methylamyl alcohol 2-ethylbutanol, n-octanol, etc.), polyvalent Alcohol or its derivatives (ethylene glycol, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, propylene glycol, propylene glycol monomethyl ether, propylene glycol monoethyl ether, triethylene glycol, 1,3-butylene glycol, hexylene glycol, etc.) , Ketones (acetone, methyl acetone, methyl ethyl ketone, methyl isobutyl ketone, methyl-n-propyl ketone, etc.), esters (ethyl acetate, acetic acid, etc.) An isopropyl, etc.), can be exemplified ethers (ethyl ether, isopropyl ether, n- butyl ether), one or two or more of them mixed solvent, of the like.
非極性溶媒としては、脂肪属炭化水素類(石油エーテル、n−ヘキサン、n−ペンタン、n−ブタン、n−オクタン、シクロヘキサン等)、四塩化炭素、クロロホルム、ジクロロメタン、トリクロロエチレン、ベンゼン、トルエン、などのうちの一種、またはこれら二種以上の混合溶媒をあげることができる。また、前記した極性溶媒と非極性溶媒の混合溶媒を用いることもできる。 Nonpolar solvents include aliphatic hydrocarbons (petroleum ether, n-hexane, n-pentane, n-butane, n-octane, cyclohexane, etc.), carbon tetrachloride, chloroform, dichloromethane, trichloroethylene, benzene, toluene, etc. One of these, or a mixed solvent of two or more of these can be mentioned. A mixed solvent of the polar solvent and the nonpolar solvent described above can also be used.
このような溶媒を用いて得られたヒュウガトウキの抽出物(以下、「ヒュウガトウキ抽出物」と称する場合もある。)が、本発明に係る皮膚または毛髪の黒化促進剤となる。 The extract of Hyugatouki obtained using such a solvent (hereinafter sometimes referred to as “Hyugatoki extract”) is the skin or hair blackening promoter according to the present invention.
(黒化促進用外用剤)
本発明に係る黒化促進用外用剤として、例えば、頭皮頭髪用製剤、皮膚用外用剤などをあげることができる。いずれの態様をとる場合であっても、有効成分であるヒュウガトウキ抽出物を含有することは言うまでもないが、養毛剤等の頭皮頭髪用製剤や、皮膚外用剤に通常用いられる成分を、本発明の効果を損なわない限り、必要に応じて適宜含有することができる。
(External preparation for promoting blackening)
Examples of external preparations for promoting blackening according to the present invention include preparations for scalp and hair, and external preparations for skin. In any case, it goes without saying that the active ingredient Hyugatoki extract is contained, but the ingredients usually used in scalp and hair preparations such as hair nourishing agents and skin external preparations are used in the present invention. As long as the effect is not impaired, it can be contained as needed.
前記した通常用いられる成分として、例えば、希釈剤(水、エタノール、イソプロピルアルコール、グリコール類等)、アニオン性界面活性剤(アルキルベンゼンスルホン酸塩、ポリオキシアルキレンアルキル硫酸エステル塩、アルキル硫酸エステル塩、オレフィンスルホン酸塩、アルキルりん酸塩、ポリオキシアルキレンアルキルエーテルりん酸塩、ジアルキルスルホコハク酸塩および脂肪酸塩等)、非イオン性界面活性剤(ポリオキシエチレンアルキルエーテル、ポリオキシエチレン脂肪酸エステル、多価アルコール脂肪酸部分エステル、ポリオキシエチレン多価アルコール脂肪酸部分エステル、ポリグリセリン脂肪酸エステル、ポリオキシエチレン硬化ヒマシ油誘導体および脂肪酸ジエタノールアミド等)、カチオン性界面活性剤(第3級脂肪族アミン塩、アルキルトリメチルアンモニウムハライド、ジアルキルジメチルアンモニウムハライドおよびアルキルジメチルベンジルアンモニウムハライド等)、両性界面活性剤(アミドベタイン型、イミダゾリニウムベタイン型およびスルホベタイン型の界面活性剤等)、高級アルコール(セチルアルコール、ステアリルアルコール、ベヘニルアルコール等)、油分(高級脂肪酸、固形パラフィン、流動パラフィン、シリコーン油、高分子シリコーンおよびその誘導体、スクワラン、ワセリン、エステル油等)、保湿剤(グリセリン、プロピレングリコール、1,3−ブチレングリコール、ジプロピレングリコールおよびソルビトール等)、増粘剤(メチルセルロース、ヒドロキシエチルセルロース、などの成分を挙げることができる。 Examples of the usually used components include diluents (water, ethanol, isopropyl alcohol, glycols, etc.), anionic surfactants (alkyl benzene sulfonates, polyoxyalkylene alkyl sulfates, alkyl sulfates, olefins). Sulfonates, alkyl phosphates, polyoxyalkylene alkyl ether phosphates, dialkyl sulfosuccinates and fatty acid salts, etc.), nonionic surfactants (polyoxyethylene alkyl ethers, polyoxyethylene fatty acid esters, polyhydric alcohols) Fatty acid partial ester, polyoxyethylene polyhydric alcohol fatty acid partial ester, polyglycerin fatty acid ester, polyoxyethylene hydrogenated castor oil derivative, fatty acid diethanolamide, etc.), cationic surfactant (No. Grade aliphatic amine salts, alkyltrimethylammonium halides, dialkyldimethylammonium halides and alkyldimethylbenzylammonium halides), amphoteric surfactants (amide betaine type, imidazolinium betaine type and sulfobetaine type surfactants, etc.), high grade Alcohol (cetyl alcohol, stearyl alcohol, behenyl alcohol, etc.), oil (higher fatty acids, solid paraffin, liquid paraffin, silicone oil, polymeric silicone and derivatives thereof, squalane, petrolatum, ester oil, etc.), moisturizer (glycerin, propylene glycol, 1,3-butylene glycol, dipropylene glycol, sorbitol, etc.) and thickeners (methyl cellulose, hydroxyethyl cellulose, etc.). That.
また、頭皮頭髪用製剤においては、養毛成分をさらに含有し、抗白髪効果と同時に養毛効果を積極的に付与することができる。
養毛成分としては、例えば、養毛効果が認められる植物抽出エキス(センブリエキス、ニンジン抽出液等)、ビタミン類(ビタミンB6、ビタミンEおよびその誘導体、ビオチン等のビタミン類)、パントテン酸およびその誘導体、グリチルリチン酸およびその誘導体、ニコチン酸エステル類(ニコチン酸ベンジル等)、アミノ酸類(セリン、メチオニン、アルギニン等)、セファランチン、塩化カプロニウム、ミノキシジル、ニコランジル、アセチルコリン誘導体、サイクロスポリン類、女性ホルモン剤(エストラジオール等)、抗菌剤(ヒノキチオール、ヘキサクロロフェン、ベンザルコニウムクロリド、セチルピリジニウムクロリド、ウンデシレン酸、トリクロロカルバニリドおよびビチオノール等)、清涼剤(メントール等)、サリチル酸、亜鉛およびその誘導体、活性物質(乳酸およびそのアルキルエステル等)、有機酸類(クエン酸等)、などを挙げることができる。
Further, the scalp and scalp hair preparation further contains a hair nourishing component, and can positively impart the hair nourishing effect simultaneously with the anti-white hair effect.
Examples of hair nourishing ingredients include plant extracts (such as assembly extract, carrot extract, etc.), vitamins (vitamin B6, vitamin E and derivatives thereof, vitamins such as biotin), pantothenic acid and Derivatives, glycyrrhizic acid and its derivatives, nicotinic acid esters (benzyl nicotinate, etc.), amino acids (serine, methionine, arginine, etc.), cephalanthin, capronium chloride, minoxidil, nicorandil, acetylcholine derivatives, cyclosporines, female hormone agents (Such as estradiol), antibacterial agents (such as hinokitiol, hexachlorophene, benzalkonium chloride, cetylpyridinium chloride, undecylenic acid, trichlorocarbanilide, and bithionol), cooling agents (such as menthol), salis Le acid, zinc and derivatives thereof, active substances (lactic acid and its alkyl esters, etc.), organic acids (such as citric acid), and the like.
なお、黒化促進用外用剤は、液剤、乳化剤、ゲル化剤、軟膏、エアゾル剤、ムース剤など、皮膚、頭皮、頭髪に塗布または浸透可能な性状のものであれば、いずれの態様をとることができる。具体的には、エモリエントローション、エモリエントクリーム、モイスチャージェル、化粧水、ヘアトニック、ヘアリキッド、スカルプトリートメント、ヘアクリーム、エアゾールムース、エアゾールスプレー、ヘアジェル、スプレームース、などと称される製品形態をとることができる。
黒化促進用外用剤におけるヒュウガトウキ抽出物の含有量は、外用剤全量中0.01〜100重量%とすることが考えられる。好ましい含有量の下限値は0.05重量%であり、0.05重量%未満であると黒化促進に対し顕著な効果がみられない。より好ましい含有量の下限値は0.1重量%であって、0.1重量%以上の含有により、さらに顕著な黒化促進効果があらわれる。なお、前記したようなその他の成分は、必要に応じて適量を含有することは言うまでも無い。
The external preparation for promoting blackening takes any form as long as it has a property that can be applied to or penetrates the skin, scalp, and hair, such as a liquid agent, an emulsifier, a gelling agent, an ointment, an aerosol agent, and a mousse agent. be able to. Specifically, it takes the form of products called emollient lotion, emollient cream, moisture gel, lotion, hair tonic, hair liquid, scalp treatment, hair cream, aerosol mousse, aerosol spray, hair gel, spray mousse, etc. Can do.
It is conceivable that the content of the Hyugatouki extract in the external preparation for promoting blackening is 0.01 to 100% by weight in the total amount of the external preparation. The lower limit of the preferred content is 0.05% by weight, and if it is less than 0.05% by weight, no significant effect on the promotion of blackening is observed. A more preferable lower limit of the content is 0.1% by weight, and when the content is 0.1% by weight or more, a further remarkable blackening promoting effect appears. In addition, it cannot be overemphasized that other components as mentioned above contain a suitable quantity as needed.
(黒化促進用飲食品)
本発明に係る黒化促進用飲食品は、人の健康危害を加えるおそれが少なく、日常生活において経口又は消化管投与などにより摂取されるものであって、例えば、一般の飲食品、健康食品、健康飲料、保健機能食品、保健機能飲料、栄養補助食品、栄養補助飲料、医薬部外品、医薬品などを含む。
また、前記したヒュウガトウキ抽出物を適量含有するものであっても良いし、ヒュウガトウキ抽出物そのものであってもよい。
(Black and white food and drink)
The food and drink for promoting blackening according to the present invention is less likely to cause human health hazards and is ingested by oral or gastrointestinal administration in daily life, for example, general food and drink, health food, Includes health drinks, health functional foods, health functional drinks, nutritional supplements, nutritional supplements, quasi-drugs, and pharmaceuticals.
Moreover, the above-mentioned Hyugatouki extract may be contained in an appropriate amount, or the Hyugatouki extract itself may be used.
黒化促進用飲食品の形態は特に限定されるものではなく、目的に応じて適宜選択することができる。例えば、飲料(清涼飲料、炭酸飲料、栄養飲料、果実飲料、乳酸飲料等)、冷菓(アイスクリーム、アイスシャーベット、かき氷等)、麺類(そば、うどん、はるさめ、中華麺、即席麺等)、餃子の皮、シュウマイの皮、菓子類(飴、キャンディー、ガム、チョコレート、錠菓、スナック菓子、ビスケット、ゼリー、ジャム、クリーム、焼き菓子、パン等)、水産物(カニ、サケ、アサリ、マグロ、イワシ、エビ、カツオ、サバ、クジラ、カキ、サンマ、イカ、アカガイ、ホタテ、アワビ、ウニ、イクラ、トコブシ等)、水産・畜産加工食品(かまぼこ、ハム、ソーセージ等)、乳製品(加工乳、発酵乳等)、油脂および油脂加工食品(乳製品、サラダ油、てんぷら油、マーガリン、マヨネーズ、ショートニング、ホイップクリーム、ドレッシング等)、調味料(ソース、たれ等)、レトルトパウチ食品(カレー、シチュー、親子丼、お粥、雑炊、中華丼、かつ丼、天丼、うな丼、ハヤシライス、おでん、マーボドーフ、牛丼、ミートソース、玉子スープ、オムライス、餃子、シュウマイ、ハンバーグ、ミートボール等)、その他、種々の形態の健康食品、健康飲料、栄養補助食品、栄養補助飲料や、錠剤、カプセル剤、ドリンク剤、トローチ等の医薬品、医薬部外品など、種々の態様を挙げることができる。 The form of the food for promoting blackening is not particularly limited, and can be appropriately selected according to the purpose. For example, beverages (soft drinks, carbonated drinks, nutrient drinks, fruit drinks, lactic acid drinks, etc.), frozen desserts (ice cream, ice sherbet, shaved ice, etc.), noodles (soba, udon, harusame, Chinese noodles, instant noodles, etc.), dumplings Skin, shumai skin, confectionery (strawberry, candy, gum, chocolate, tablet confectionery, snack confectionery, biscuits, jelly, jam, cream, baked confectionery, bread, etc.), seafood (crab, salmon, clams, tuna, sardines, Shrimp, skipjack, mackerel, whale, oyster, saury, squid, red scallop, scallop, abalone, sea urchin, salmon roe, tocobushi, etc., fishery and livestock processed foods (kamaboko, ham, sausage, etc.), dairy products (processed milk, fermented milk) Etc.), fats and oils and processed foods (dairy products, salad oil, tempura oil, margarine, mayonnaise, shortening, whipped cream, dress ), Seasonings (sauce, sauce, etc.), retort pouch foods (curry, stew, oyakodon, rice bowl, miscellaneous rice, Chinese rice bowl, bonito, tempura, eel rice, hayashi rice, oden, mabodorf, beef bowl, meat sauce, Egg soup, omelet rice, dumplings, shumai, hamburger, meatballs, etc.), various other forms of health foods, health drinks, nutritional supplements, nutritional supplements, and pharmaceuticals such as tablets, capsules, drinks, troches, Various aspects such as quasi-drugs can be exemplified.
黒化促進用飲食品におけるヒュウガトウキ抽出物の含有量は、対象となる飲食品の種類に応じて異なるため、必ずしも一概には規定することはできない。
例えば、飲食品本来の味を損なわない範囲で含有することを目的とした場合、ヒュウガトウキ抽出物の含有量を0.001〜50重量%とすることが考えられる。好ましい含有量の下限値は0.1重量%であり、0.1重量%未満であると黒化促進に対し顕著な効果がみられない。より好ましい含有量の下限値は0.15重量%であって、0.15重量%以上の含有により、さらに顕著な黒化促進効果があらわれる。
また、顆粒、錠剤、カプセル、ドリンク剤などの形態とする場合には、ヒュウガトウキ抽出物の含有量を0.01〜100重量%とすることが考えられ、5〜100重量%とすることがより好ましい。
Since the content of the Hyugatouki extract in the food for promoting blackening differs depending on the type of food or drink to be targeted, it cannot always be specified unconditionally.
For example, when it aims at containing in the range which does not impair the original taste of food / beverage products, it is possible to make content of a Hyugatouki extract 0.001-50 weight%. The lower limit of the preferred content is 0.1% by weight, and if it is less than 0.1% by weight, no significant effect on the promotion of blackening is observed. A more preferable lower limit of the content is 0.15% by weight, and when the content is 0.15% by weight or more, an even more significant blackening promoting effect appears.
Moreover, when it is set as the form of a granule, a tablet, a capsule, a drink, etc., it is possible to make content of a Hyugatouki extract into 0.01 to 100 weight%, and it is set as 5 to 100 weight%. More preferred.
次に、試料を用いた試験例および実施例について述べるが、本発明はこれら試料、試験例、実施例などに限定されるものではない。 Next, test examples and examples using samples will be described, but the present invention is not limited to these samples, test examples, and examples.
(試験例1:細胞培養によるメラニン色素の増殖率の比較)
(ヒュウガトウキ抽出物の調製)
まず、乾燥したヒュウガトウキの葉部および茎部50gを、水:1,3ブチレングリコール(1:1)溶液1Lにて、80〜100℃で煮出して抽出操作を行い、約500mLのヒュウガトウキ抽出物を得た。
(Test Example 1: Comparison of melanin growth rate by cell culture)
(Preparation of Hyugatouki extract)
First, 50 g of dried Hyugatouki leaves and stems were extracted with 1 L of water: 1,3 butylene glycol (1: 1) solution at 80 to 100 ° C., and about 500 mL of Hyugatouki was extracted. I got a thing.
(細胞の培養と細胞数の調整)
次に、マウスメラノーマ細胞(B16細胞)を細胞培養用シャーレ内に、細胞数が1mLあたり1×105となるよう播種し、37℃、5%−CO2の条件下で培養器内で一晩培養(前培養)した。
ここに、上記ヒュウガトウキ抽出物を、含有量がそれぞれ0.05重量%(試料1)、0.10重量%(試料2)、0.20重量%(試料3)となるよう添加し、さらに同一条件下で72時間培養した(本培養)。
培養後、各試料をトリプシン処理をして細胞を剥離させ、遠心操作により細胞を回収し、前記それぞれの含有量ごとの細胞数を細胞数が1mLあたり1×106個になるようカウントして、調整した。
他方、コントロール群(比較例1)として、1,3−ブチレングリコールを含有量0.20重量%となるよう添加したものを前記と同一条件で用意し、前記同様にして細胞数をカウントし、同一数となるよう調整した。
(Cell culture and cell number adjustment)
Next, mouse melanoma cells (B16 cells) are seeded in a petri dish for cell culture so that the number of cells is 1 × 10 5 per 1 mL, and the cells are cultured in a culture vessel under conditions of 37 ° C. and 5% CO 2. Evening culture (preculture) was performed.
Here, the above Hyugatouki extract was added so that the contents were 0.05% by weight (Sample 1), 0.10% by weight (Sample 2), and 0.20% by weight (Sample 3), respectively. Culture was performed for 72 hours under the same conditions (main culture).
After incubation, trypsinize each sample to detach the cells, collect the cells by centrifugation, and count the number of cells for each content so that the number of cells is 1 × 10 6 per mL. ,It was adjusted.
On the other hand, as a control group (Comparative Example 1), prepared by adding 1,3-butylene glycol to a content of 0.20% by weight under the same conditions as described above, counting the number of cells in the same manner as described above, It adjusted so that it might become the same number.
(メラニン色素の増殖率の評価)
次に、前記したように細胞数を調整した試料1〜3および比較例1における各マウスメラノーマ細胞についてメラニン色素の増殖率(比較例1に対する各試料の割合)を示す。
細胞数を調整したのち、前記試料1〜3および比較例1について、マイクロプレートリーダー(分光光度計)にて細胞溶解液のメラニン色素の吸光度をメラニン色素の吸収帯である405nmの波長にて測定した。測定数は、各試料とも7回の培養の平均を取った。メラニン色素の生合成が促進され増殖する度合いが大きいほど吸光度が高くなるため、試料1〜3について、比較例1を100%とした場合の相対値を「メラニン色素の増殖率」として表1および図1に示す。同表に示されるように、有意水準p=5%で、試料2と試料3は、比較例1に対して有意差があった。また、ヒュウガトウキ抽出物の濃度が増えるに従って増殖率が高くなることが確認された。
(Evaluation of growth rate of melanin pigment)
Next, the growth rate of melanin pigment (ratio of each sample with respect to Comparative Example 1) is shown for each of the mouse melanoma cells in Samples 1 to 3 and Comparative Example 1 in which the number of cells was adjusted as described above.
After adjusting the number of cells, with respect to Samples 1 to 3 and Comparative Example 1, the absorbance of the melanin pigment in the cell lysate was measured with a microplate reader (spectrophotometer) at a wavelength of 405 nm, which is the absorption band of the melanin pigment. did. The number of measurements was the average of 7 cultures for each sample. As the biosynthesis of melanin pigment is promoted and the degree of proliferation increases, the absorbance increases. Therefore, for Samples 1 to 3, the relative value when Comparative Example 1 is 100% is defined as “growth rate of melanin pigment” and Table 1 As shown in FIG. As shown in the table, Sample 2 and Sample 3 were significantly different from Comparative Example 1 at the significance level p = 5%. It was also confirmed that the growth rate increased as the concentration of Hyugatouki extract increased.
(色調による評価)
前記試料1〜3および比較例1について、前記のように細胞数の調整をした細胞を1mol/LのNaOH溶液で溶解し、色調の変化を目視により観察した。濃くなっている場合は+、より濃くなっている場合は++、さらに濃くなっている場合は+++として評価した。結果を表2に示す。この結果、ヒュウガトウキ抽出物の濃度が増えるに従って色調が濃くなることが確認された。
(Evaluation by color tone)
For Samples 1 to 3 and Comparative Example 1, the cells with the cell number adjusted as described above were dissolved in a 1 mol / L NaOH solution, and the change in color tone was visually observed. When it was dark, it was evaluated as +, when it was darker, ++, and when it was darker, it was evaluated as +++. The results are shown in Table 2. As a result, it was confirmed that the color tone became deeper as the concentration of Hyugatouki extract increased.
(試験例2:塗布によるメラニン色素の増殖率の比較)
(ヒュウガトウキ抽出物の調製)
まず、試験例1と同様に、乾燥したヒュウガトウキの葉部および茎部50gを、水:1,3ブチレングリコール(1:1)溶液1Lにて、80〜100℃で煮出して抽出操作を行い、約500mLのヒュウガトウキ抽出物を得た。このヒュウガトウキ抽出物を、含有量がそれぞれ0.10重量%(試料4)、1.00重量%(試料5)、10.0重量%(試料6)となるよう、1%キサンタンガムゲルに添加してゲル状の試料4、5、6とした。
(Test Example 2: Comparison of proliferation rate of melanin pigment by application)
(Preparation of Hyugatouki extract)
First, as in Test Example 1, 50 g of dried Hyugatouki leaves and stems were boiled at 80 to 100 ° C. in 1 L of a water: 1,3 butylene glycol (1: 1) solution, and an extraction operation was performed. About 500 mL of Hyugatouki extract was obtained. This Hyugatouki extract was added to 1% xanthan gum gel so that the contents would be 0.10 wt% (Sample 4), 1.00 wt% (Sample 5), 10.0 wt% (Sample 6), respectively. Thus, the gel samples 4, 5, and 6 were obtained.
(反復塗布)
次に、上記試料4〜6を、背部毛を刈り取り採取したマウス(C57BL/6)の背部に3週間にわたり反復塗布した。3週間後、再び生えた背部毛を刈り取り採取した。
他方、比較例2として、キサンタンガム100%のゲルを用い、前記と同一条件で同一量の背部毛を刈り取り採取した。
(Repeated application)
Next, the above samples 4 to 6 were repeatedly applied to the back of a mouse (C57BL / 6) from which the back hair was cut and collected for 3 weeks. Three weeks later, the growing back hair was cut and collected.
On the other hand, as Comparative Example 2,
(メラニン色素の増殖率の評価)
次に、前記試料4〜6および比較例2における塗布後の背部毛ついて、1mol/LのNaOH溶液で溶解し、マイクロプレートリーダー(分光光度計)にてその溶解液のメラニン色素の吸光度をメラニン色素の吸収波長帯である405nmの波長にて測定した。測定数は、各試料とも5回の培養の平均を取った。メラニン色素の生合成が促進され増殖する度合いが大きいほど吸光度が高くなるため、試料4〜6について、比較例2を100%とした場合の相対値を「メラニン色素の増殖率」として表3および図2に示す。同表に示されるように、有意水準p=5%で、試料5と試料6は比較例2に対して有意差があった。また、ヒュウガトウキ抽出物の濃度が増えるに従って増殖率が高くなることが確認された。
(Evaluation of growth rate of melanin pigment)
Next, the back hair after application in Samples 4 to 6 and Comparative Example 2 was dissolved in a 1 mol / L NaOH solution, and the absorbance of the melanin pigment in the solution was measured with a microplate reader (spectrophotometer). The measurement was performed at a wavelength of 405 nm which is an absorption wavelength band of the dye. The number of measurements was the average of five cultures for each sample. As the biosynthesis of melanin pigment is promoted and the degree of proliferation increases, the absorbance increases. Therefore, with respect to Samples 4 to 6, the relative value when Comparative Example 2 is 100% is defined as “growth rate of melanin pigment” in Table 3 and As shown in FIG. As shown in the table, Sample 5 and Sample 6 were significantly different from Comparative Example 2 at the significance level p = 5%. It was also confirmed that the growth rate increased as the concentration of Hyugatouki extract increased.
(色調による評価)
前記試料6および比較例2における塗布前と塗布後の背部毛ついて、1mol/LのNaOH溶液で細胞を溶解したものの色調の変化を目視により観察したところ、比較例2では変化が見られず、試料6では塗布後に色調が濃くなることが確認された(表4参照)。
(Evaluation by color tone)
Regarding the back hair before and after application in Sample 6 and Comparative Example 2, when the cells were dissolved with a 1 mol / L NaOH solution, the color tone was visually observed. In Comparative Example 2, no change was observed. In sample 6, it was confirmed that the color tone became dark after application (see Table 4).
(試験例3:経口投与によるメラニン色素の増殖率の比較)
(ヒュウガトウキ抽出物の調製)
まず、乾燥したヒュウガトウキの葉部および茎部30gを、80〜100℃の熱湯で煮出して抽出操作を行い、ヒュウガトウキ抽出物を得た。さらにこのヒュウガトウキ抽出物を、含有量がそれぞれ0.10重量%(試料7)、0.15重量%(試料8)、1.50重量%(試料9)となるよう乳糖にて賦形し、それぞれが約20gとなるよう粉末状の試料7、8、9を得た。
(Test Example 3: Comparison of growth rate of melanin by oral administration)
(Preparation of Hyugatouki extract)
First, 30 g of dried Hyugatouki leaves and stems were boiled in hot water at 80 to 100 ° C. to perform an extraction operation to obtain a Hyugatouki extract. Further, this Hyugatouki extract was shaped with lactose so that the contents were 0.10 wt% (Sample 7), 0.15 wt% (Sample 8), and 1.50 wt% (Sample 9), respectively. , Powdered samples 7, 8, and 9 were obtained so that each would be about 20 g.
(反復投与)
次に、前記試料7〜9を水に溶かしたものを、背部毛を刈り取り採取したマウス(C57BL/6)に対し、3週間にわたり自由摂取にて投与した。3週間後に再び生えた背部毛を刈り取り採取した。
他方、比較例3として水のみを与えた。
(Repeated administration)
Next, the sample 7-9 dissolved in water was administered to a mouse (C57BL / 6) from which the back hair was cut and collected for 3 weeks. After 3 weeks, the back hair that had grown again was cut and collected.
On the other hand, as Comparative Example 3, only water was given.
次に、前記試料7〜9および比較例3における投与後の背部毛について、1mol/LのNaOH溶液で溶解し、マイクロプレートリーダーにてその溶解液のメラニン色素の吸光度をメラニン色素の吸収波長帯である405nmの波長にて測定した。測定数は、各試料とも5回の培養の平均を取った。メラニン色素の生合成が促進され増殖する度合いが大きいほど吸光度が高くなるため、試料4〜6について、比較例を100%とした場合の相対値を「メラニン色素の増殖率」として表5および図3に示す。同表に示されるように、有意水準p=5%で、試料8と試料9は比較例3に対して有意差があった。また、ヒュウガトウキ抽出物の濃度が増えるに従って増殖率が高くなることが確認された。 Next, the dorsal hair after administration in Samples 7 to 9 and Comparative Example 3 was dissolved in a 1 mol / L NaOH solution, and the absorbance of the melanin pigment in the solution was measured with a microplate reader using the absorption wavelength band of the melanin pigment. Measured at a wavelength of 405 nm. The number of measurements was the average of five cultures for each sample. As the biosynthesis of melanin pigment is promoted and the degree of proliferation increases, the absorbance increases. Therefore, for Samples 4 to 6, Table 5 and FIG. 3 shows. As shown in the table, Sample 8 and Sample 9 were significantly different from Comparative Example 3 at the significance level p = 5%. It was also confirmed that the growth rate increased as the concentration of Hyugatouki extract increased.
(色調による評価)
前記試料9および比較例3における投与前と投与後の背部毛ついて、1mol/LのNaOH溶液で溶解したものの色調の変化を目視により観察したところ、比較例3では変化が見られず、試料9では投与後に色調が濃くなることが確認された(表6参照)。
(Evaluation by color tone)
When the change in color tone of the back hair before and after administration in Sample 9 and Comparative Example 3 dissolved in a 1 mol / L NaOH solution was visually observed, no change was observed in Comparative Example 3, and Sample 9 Then, it was confirmed that the color tone became darker after administration (see Table 6).
以上の結果から、本発明に係る黒化促進剤、黒化促進用外用剤、黒化促進用飲食品において、所望の黒化促進効果を認められることが確認できた。 From the above results, it was confirmed that the blackening accelerator, the external preparation for promoting blackening, and the food for food and drink for promoting blackening according to the present invention have a desired blackening promoting effect.
以下、より詳細な実施例について述べる。
(実施例1:毛髪の黒化促進外用剤としての毛髪用黒化促進ローション)
ヒュウガトウキ抽出物、ポリオキシエチレンジオレイン酸メチルグルコシド(界面活性剤)、L−メントール(浸透促進剤)、防腐剤、香料を60℃で加熱溶解したものを、精製水と共に混合しホモミキサー処理して、各成分の含有割合が下記のとおりである毛髪用黒化促進ローションを得た。
ヒュウガトウキ抽出物 10重量%
ポリオキシエチレンジオレイン酸メチルグルコシド 0.2重量%
L−メントール 0.2重量%
防腐剤 0.2重量%
香料 0.1重量%
精製水 残 部
Hereinafter, more detailed examples will be described.
(Example 1: Hair blackening promoting lotion as a hair blackening promoting external preparation)
Hyugatouki extract, polyoxyethylene dioleic acid methyl glucoside (surfactant), L-menthol (penetration enhancer), preservative, fragrance, heated and dissolved at 60 ° C, mixed with purified water and homomixed And the blackening acceleration | stimulation lotion for hair whose content rate of each component is as follows was obtained.
Hyugatouki extract 10% by weight
Polyoxyethylene dioleic acid methyl glucoside 0.2% by weight
L-menthol 0.2% by weight
Preservative 0.2% by weight
Fragrance 0.1% by weight
Purified water balance
(実施例2:皮膚の黒化促進外用剤としての皮膚用黒化促進クリーム)
ステアリン酸ナトリウム、モノステアリン酸ポリオキシエチレンソルビタン(20EO)、ベヘニルアルコール、自己乳化型モノステアリン酸グリセリンを75℃で加熱溶解し混合してホモミキサー処理したものをA相(油相)とし、ヒュウガトウキ抽出物、濃グリセリン、1,3−ブチレングリコール、防腐剤、香料を加熱溶解し精製水と共に混合してホモミキサー処理したものをB相(水相)とし、さらにこれらA相とB相を混合して、各成分の含有割合が下記のとおりである皮膚用黒化促進クリームを得た。
(A相)
ステアリン酸ナトリウム 5重量%
モノステアリン酸ポリオキシエチレンソルビタン 3重量%
ベヘニルアルコール 2重量%
自己乳化型モノステアリン酸グリセリン 3重量%
(B相)
ヒュウガトウキ抽出物 10重量%
濃グリセリン 5重量%
1,3−ブチレングリコール 5重量%
防腐剤 0.2重量%
香料 0.2重量%
精製水 残 部
(Example 2: Skin darkening promoting cream as an external preparation for promoting skin darkening)
Sodium stearate, polyoxyethylene sorbitan monostearate (20EO), behenyl alcohol, self-emulsifying type glyceryl monostearate heated and dissolved at 75 ° C., mixed and treated with a homomixer to make A phase (oil phase), The extract, concentrated glycerin, 1,3-butylene glycol, preservative, and fragrance are heated and dissolved, mixed with purified water and treated with a homomixer to make a B phase (aqueous phase), and these A and B phases are mixed. Thus, a skin darkening promoting cream having the following content ratio of each component was obtained.
(Phase A)
Sodium stearate 5% by weight
3% by weight polyoxyethylene sorbitan monostearate
2% by weight of behenyl alcohol
Self-emulsifying glyceryl monostearate 3% by weight
(Phase B)
Hyugatouki extract 10% by weight
Concentrated glycerin 5% by weight
1,3-butylene glycol 5% by weight
Preservative 0.2% by weight
Fragrance 0.2% by weight
Purified water balance
(実施例3:皮膚の黒化促進剤としての皮膚用黒化促進ジェル)
カルボキシビニルポリマー、濃グリセリン、1,3−ブチレングリコールを60〜75℃で加熱溶解し混合してホモミキサー処理したものをA相(油相)とし、ヒュウガトウキ抽出物、防腐剤、香料を60〜75℃で加熱溶解し精製水と共に混合してホモミキサー処理したものをB相(水相)とし、さらにA相にB相を添加して、各成分の含有割合が下記のとおりである皮膚用黒化促進ジェルを得た。
(A相)
カルボキシビニルポリマー 1重量%
濃グリセリン 5重量%
1,3−ブチレングリコール 5重量%
(B相)
ヒュウガトウキ抽出物 10重量%
防腐剤 0.2重量%
香料 0.2重量%
精製水 残 部
(Example 3: Skin darkening promoting gel as a skin darkening accelerator)
Carboxyvinyl polymer, concentrated glycerin, and 1,3-butylene glycol are heated and dissolved at 60 to 75 ° C., mixed and homomixed, and treated as a phase A (oil phase). Hyugatouki extract, preservative and flavoring agent are 60 Skin heated and dissolved at ˜75 ° C., mixed with purified water and treated with a homomixer to form B phase (aqueous phase), and further, B phase is added to A phase, and the content ratio of each component is as follows A blackening promoting gel was obtained.
(Phase A)
Carboxy vinyl polymer 1% by weight
Concentrated glycerin 5% by weight
1,3-butylene glycol 5% by weight
(Phase B)
Hyugatouki extract 10% by weight
Preservative 0.2% by weight
Fragrance 0.2% by weight
Purified water balance
(実施例4:皮膚、毛髪の黒化促進用飲食品としての錠剤状栄養補助食品)
それぞれ粉末状としたヒュウガトウキ抽出物、セルロース末、ショ糖脂肪酸エステルを60〜75℃で加熱溶解したものを、乳糖(賦形剤)と共に混合しホモミキサー処理した後、錠剤状に成型して、各成分の含有割合が下記のとおりである錠剤状栄養補助食品を得た。
ヒュウガトウキ抽出物 1.5重量%
乳糖 53.5重量%
セルロース末 44重量%
ショ糖脂肪酸エステル 1重量%
(Example 4: Tablet-like dietary supplement as food and drink for promoting blackening of skin and hair)
Each powdered Hyugatouki extract, cellulose powder, and sucrose fatty acid ester heated and dissolved at 60 to 75 ° C. are mixed with lactose (excipient), homomixed and processed into tablets. The tablet-like nutritional supplement whose content rate of each component is as follows was obtained.
Hyugatouki extract 1.5% by weight
Lactose 53.5% by weight
Cellulose powder 44% by weight
Sucrose fatty acid ester 1% by weight
(実施例5:皮膚、毛髪の黒化促進用飲食品としての顆粒状栄養補助食品)
それぞれ粉末状としたヒュウガトウキ抽出物、デキストリン、クエン酸を60〜75℃で加熱溶解したものを、ブドウ糖(賦形剤)と共に混合しホモミキサー処理した後、粉末状に成形して、各成分の含有割合が下記のとおりである顆粒状栄養補助食品を得た。
ヒュウガトウキ抽出物 1.5重量%
ブドウ糖 35重量%
デキストリン 58.5重量%
クエン酸 5重量%
(Example 5: Granular dietary supplement as food and drink for promoting skin and hair blackening)
Each of the powdered Hyugatouki extract, dextrin, and citric acid, heated and dissolved at 60-75 ° C., is mixed with glucose (excipient), homomixed, and then molded into powder form. A granular dietary supplement having the following content ratio was obtained.
Hyugatouki extract 1.5% by weight
Glucose 35% by weight
Dextrin 58.5% by weight
Citric acid 5% by weight
これら各実施例についても前記試験例と同様の試験を行い、前記と同様の結果が得られることは確認済みである。
以上、本発明の実施の形態について、試料、試験例、実施例などをあげて説明したが、本発明は上記した実施の形態に限定されるものではなく、発明の要旨を変えない範囲で変更可能であることは言うまでもない。
For each of these examples, the same test as in the above test example was conducted, and it was confirmed that the same result as above was obtained.
The embodiments of the present invention have been described with reference to samples, test examples, examples, and the like, but the present invention is not limited to the above-described embodiments, and changes can be made without changing the gist of the invention. It goes without saying that it is possible.
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