KR100797366B1 - Cosmetic composition containing Liquidambar taiwaniana Hance extracts and Cynanchum atratum Bunge extracts - Google Patents

Cosmetic composition containing Liquidambar taiwaniana Hance extracts and Cynanchum atratum Bunge extracts Download PDF

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KR100797366B1
KR100797366B1 KR1020000059995A KR20000059995A KR100797366B1 KR 100797366 B1 KR100797366 B1 KR 100797366B1 KR 1020000059995 A KR1020000059995 A KR 1020000059995A KR 20000059995 A KR20000059995 A KR 20000059995A KR 100797366 B1 KR100797366 B1 KR 100797366B1
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extract
roroton
white rice
extracts
cosmetic composition
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KR20020029181A (en
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김호정
진무현
김청택
김원찬
강상진
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주식회사 엘지생활건강
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    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K8/00Cosmetics or similar toiletry preparations
    • A61K8/18Cosmetics or similar toiletry preparations characterised by the composition
    • A61K8/96Cosmetics or similar toiletry preparations characterised by the composition containing materials, or derivatives thereof of undetermined constitution
    • A61K8/97Cosmetics or similar toiletry preparations characterised by the composition containing materials, or derivatives thereof of undetermined constitution from algae, fungi, lichens or plants; from derivatives thereof
    • A61K8/9783Angiosperms [Magnoliophyta]
    • A61K8/9789Magnoliopsida [dicotyledons]
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61QSPECIFIC USE OF COSMETICS OR SIMILAR TOILETRY PREPARATIONS
    • A61Q19/00Preparations for care of the skin
    • A61Q19/02Preparations for care of the skin for chemically bleaching or whitening the skin
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K2800/00Properties of cosmetic compositions or active ingredients thereof or formulation aids used therein and process related aspects
    • A61K2800/80Process related aspects concerning the preparation of the cosmetic composition or the storage or application thereof
    • A61K2800/84Products or compounds obtained by lyophilisation, freeze-drying

Abstract

본 발명은 멜라닌 생성 억제 효과가 우수한 로로통 추출물, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물에 관한 것이다.The present invention relates to a cosmetic composition containing, as an active ingredient, at least one selected from roroton extract and white rice extract excellent in melanin production inhibitory effect.

본 발명의 로로통, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물은 미백 효과 및 색소 침착 저해 효과를 보이며 피부내에서 어떤 부작용도 나타나지 않아 안전하고 기미나 주근깨 개선효과가 우수하다.


Cosmetic composition containing at least one selected from Roroton, white rice extract of the present invention as an active ingredient shows a whitening effect and pigmentation inhibitory effect and does not show any side effects in the skin and is safe and excellent in improving freckles and freckles. .


로로통, 백미, 미백효과, 기미, 주근깨 Roroton, white rice, whitening effect, blemish, freckles

Description

로로통 추출물, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물{Cosmetic composition containing Liquidambar taiwaniana Hance extracts and Cynanchum atratum Bunge extracts}Cosmetic composition containing at least one selected from Roroton extract, white rice extract as an active ingredient {Cosmetic composition containing Liquidambar taiwaniana Hance extracts and Cynanchum atratum Bunge extracts}

본 발명은 로로통 추출물, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물에 관한 것으로서, 보다 상세하게는 본 발명은 멜라닌 생성 억제 효과가 우수한 로로통 추출물, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물에 관한 것이다.The present invention relates to a cosmetic composition containing at least one selected from roroton extract, white rice extract as an active ingredient, and more particularly, the present invention is selected from roroton extract, white rice extract excellent in melanin production inhibitory effect. It relates to a cosmetic composition containing at least a species as an active ingredient.

희고 고운 피부를 갖고자 하는 것은 모든 사람의 한결같은 소망이다. 사람의 피부색은 피부내 멜라닌(melanin)의 농도와 분포에 따라 유전적으로 결정되나, 태양 자외선이나 피로, 스트레스 등의 환경적 또는 생리적 조건에 의해서도 영향을 받는다. 멜라닌은 아미노산의 일종인 티로신(tyrosine)에 티로시나제(tyrosinase)라는 효소가 작용하여 도파(DOPA), 도파퀴논(dopaquinone)으로 바뀐 후 비효소적인 산화반응을 거쳐 만들어 진다. 그러나 멜라닌이 만들어지는 경로는 알려져 있으나, 티로시나제가 작용하는 이전 단계인 멜라닌 합성을 유도하는 메카니즘(mechanism)이 무엇인지에 대해서는 아직도 자세히 밝혀지지 않고 있다. 한편 멜라닌 색소의 합성을 저해함으로서 피부 톤을 밝게하여 피부 미백을 실현할 수 있을뿐만 아니라 자외선, 호르몬, 유전에 기인한 기미, 자외선, 유전에 기인한 주근깨 등의 피부 과색소 침착증의 개선이 가능하다. 이에 종래에는 하이드로퀴논(hydroquinone)이나 아스콜빈산(ascorbic acid), 고지산(kojic acid), 글루타치온(glutathione)같은 티로시나제에 저해 활성을 갖는 물질을 연고나 화장료에 배합하여, 피부 미백이나 기미, 주근깨 개선의 목적에 사용하여 왔으나, 하이드로퀴논의 미백효과는 인정되지만 피부자극성이 심하여 사용량이 극히 제한된다. 또한 아스콜빈산은 산화되기 쉬워 이를 배합한 화장료는 변색, 변취되는 등의 문제를 야기하며 글루타치온, 시스테인 등의 티올계 화합물은 특유의 불쾌한 냄새가 나며 경피흡수에 문제가있다. 또한 이들의 배당체 및 유도체들은 극성이 높아 화장료의 배합 성분으로 사용하기에는 문제가 있다. 또한 태반 추출물 등은 미백 효과가 불충분하다는 문제가 있다.It is everyone's constant desire to have white, fair skin. Human skin color is genetically determined by the concentration and distribution of melanin in the skin, but is also influenced by environmental or physiological conditions such as solar ultraviolet rays, fatigue and stress. Melanin is a type of amino acid tyrosine (tyrosine) enzymes called tyrosinase (tyrosinase) acts to convert to dopa (DOPA), dopaquinone (dopaquinone) is produced through a non-enzymatic oxidation reaction. However, although the pathway by which melanin is made is known, it is still unknown in detail the mechanism by which tyrosinase acts, the mechanism that induces melanin synthesis. On the other hand, by inhibiting the synthesis of melanin pigments can not only realize skin whitening by brightening the skin tone, but also improve the hyperpigmentation of skin such as ultraviolet rays, hormones, blemishes caused by heredity, ultraviolet rays, freckles due to heredity. Therefore, conventionally, substances having inhibitory activity against tyrosinase, such as hydroquinone, ascorbic acid, kojic acid, and glutathione, are incorporated into ointments or cosmetics, and thus whitening, blemishes, and freckles of skin. Although it has been used for the purpose of improvement, the whitening effect of hydroquinone is recognized, but the amount of use is extremely limited due to severe skin irritation. In addition, ascorbic acid is easily oxidized, and the cosmetics containing the same cause problems such as discoloration and deodorization, and thiol-based compounds such as glutathione and cysteine have a characteristic unpleasant odor and have problems with transdermal absorption. In addition, these glycosides and derivatives have a high polarity, so there is a problem to use them as a component of a cosmetic. In addition, placenta extract has a problem that the whitening effect is insufficient.

로로통은 금루매과의 식물인 풍향 Liquidambar taiwaniana Hance의 열매로 맛은 씁쓸하고 떫으며 성은 평하며 독이 없다. 로로통는 거풍통락하고 이수제습하는 효능이 있으며 손발경련, 위통, 수종, 무월경, 악창, 옴, 습진을 치료하는데 사용하였다.(중약대사전) 로로통 추출물을 포함하는 보습용 화장료 조성물에 대한 연구가 있으나(JP08268837) 본 발명과는 무관하다.Roroton is the fruit of the wind berry, Liquidambar taiwaniana Hance, which is a medicinal herb. Roroton has the effect of swelling and dehumidifying and has been used to treat hand and foot cramps, stomach pain, edema, amenorrhea, swelling, scabies and eczema (Chinese medicine dictionary). (JP08268837) It is irrelevant to the present invention.

백미는 박주가리과에 속하는 다년생 초본으로 라틴명은 Radix Cynanchi Atrati이고 학명은 Cynanchum atratum Bunge. 로서 맛은 짜고 성질은 한하며 독이없다. 또한 백미는 열을 내리고 혈을 식히는 효능이 있으며 해열, 이뇨, 소종 풍습통 등을 치료한다(중약대사전, 원색약물대사전) 로로통의 성분연구에 의하면 Atratogenin A, B, (Zhongguo Zhongyao Zazhi (1989), 14(3), 138-42), 및 Glaucogenin A, C, H 및 Cynatratoside F(I)이 분리 보고 된바 있다(Chem. Pharm. Bull. (1985), 33(10), 4188-92)White rice is a perennial herb belonging to the family Ju-Ki, with Latin name Radix Cynanchi Atrati and scientific name Cynanchum atratum Bunge. The taste is salty, the nature is limited and nontoxic. In addition, white rice has the effect of lowering heat, cooling blood, and treating antipyretic, diuretic, and small-scale customary pains (Chinese medicine dictionary, primary drug drug dictionary). , 14 (3), 138-42), and Glaucogenin A, C, H and Cynatratoside F (I) have been reported separately (Chem. Pharm. Bull. (1985), 33 (10), 4188-92)

따라서, 본 발명자들은 멜라닌 합성 유도 자체를 억제하는 물질까지 스크리닝(screening)할 수 있는 쥐의 멜라노마 세포(B16 mouse melanoma cell)를 이용하여 천연에서 자생하는 동식물들을 대상으로 새로운 미백제를 개발하고자, 연구를 거듭한 결과, 로로통 추출물, 백미 추출물에 매우 강력한 멜라닌 생성 억제 효과와 미백 효과가 있음을 밝혀내어 본 발명을 완성하게 되었다.Therefore, the present inventors have attempted to develop a new whitening agent for native animals and plants using B16 mouse melanoma cells that can screen for substances that inhibit melanin synthesis induction itself. As a result, Loroton extract, white rice extract was found to have a very strong melanin production inhibitory effect and whitening effect to complete the present invention.

본 발명은 약재로 구입할 수 있는 로로통, 백미를 탄소수 1-4개의 무수 또는 함수 저급알코올 또는 에틸아세테이트 또는 아세톤 등의 유기용매로 1차 추출한 후 감압 농축한 다음 동결건조하거나 분무건조하여 1차 추출물을 제조하였다. 이러한 방법으로 제조된 로로통, 백미 추출물은 쥐의 멜라노마 세포(B-16 mouse melanoma cell)에서 매우 강력한 멜라닌 합성 저해 효과를 나타낸다. 또한 건조된 로로통, 백미추출물로 피부외용 연고나 화장료를 제조하여 사람의 피부에 도포하였을 때, 피부 미백 효과가 매우 우수하다. In the present invention, the Rorotong, white rice, which can be purchased as a medicine, is first extracted with an organic solvent such as anhydrous or hydrous lower alcohol having 1 to 4 carbon atoms or ethyl acetate or acetone, and then concentrated under reduced pressure, followed by freeze-drying or spray-drying. Was prepared. Roroton, white rice extract prepared by this method has a very potent melanin synthesis inhibitory effect in B-16 mouse melanoma cells. In addition, when the dermal ointment or cosmetics with dried Roroton, white rice extract is applied to human skin, the skin whitening effect is very excellent.

본 발명을 상세하게 설명하면 다음과 같다.The present invention will be described in detail as follows.

생약재로 시판되는 로로통, 백미를 구입하여 잘게 분쇄하고 분쇄물 건조 중량에 대하여 5-20부피의 물이나, 탄소수 1-4개의 무수 또는 함수 저급알코올, 에틸 아세테이트 또는 아세톤으로 환류 냉각기가 달린 추출기에서 50-100oC로 1-5시간 가열하여 추출한다. 여과포로 여과한 후 잔사를 같은 방법으로 1회이상씩 더 추출한다. 추출액을 합하여 감압농축한 후 동결건조나 분무 건조하여 건조추출물을 얻는다. Roroton, white rice, commercially available, is crushed and ground in an extractor equipped with a reflux condenser with 5-20 volumes of water or 1-4 anhydrous or hydrous lower alcohols, ethyl acetate or acetone, by weight of the dry matter. Extract by heating to 50-100 o C for 1-5 hours. After filtering with filter cloth, the residue is extracted one more time in the same manner. The extracts were combined and concentrated under reduced pressure, followed by freeze drying or spray drying to obtain a dry extract.

건조된 로로통, 백미 추출물을 쥐의 멜라노마 세포(B-16 melanoma cell)에 처리하였을 때, 매우 강력한 멜라닌 합성 저해효과를 나타내었다.When the dried Roroton and white rice extracts were treated with rat melanoma cells (B-16 melanoma cells), they showed very potent melanin synthesis inhibitory effects.

상기와 같이 얻어진 로로통, 백미 추출물을 함유하는 피부외용연고나 로션같은 여러 화장료를 제조한다. 로로통, 백미 추출물을 함유한 피부 외용연고나 로션 등의 화장료를 제조하여 사람의 피부에 도포하였을 때 피부 미백 효과가 매우 우수하였다. 또한 어떤 부작용도 발생하지 않아 로로통, 백미 추출물이 안전하고 효과가 매우 뛰어난 기미나 주근깨 개선 및 피부 미백제임을 알 수 있다.Various cosmetics, such as a skin external ointment or lotion containing Roroton and white rice extract obtained as described above are prepared. Skin cosmetics such as roroton and white rice extracts, such as external application ointments and lotions were prepared and applied to human skin, and the skin whitening effect was very excellent. In addition, it does not cause any side effects, so Roroton, white rice extract is a safe and very effective blemishes and freckles improvement and skin whitening agent.

피부외용연고나 화장료 제조시에 함유되는 로로통, 백미 추출물의 함량은 건조 중량으로 0.0001-10.0중량%, 바람직하게는 0.0005-10.0중량%가 적당하다. 0.0001중량%이하의 농도에서는 뚜렷한 효과를 기대할 수 없었고, 10중량%이상의 농도에서는 함유량의 증가에 따라 뚜렷한 효과의 증가가 나타나지 않았다.The content of Roroton and white rice extracts included in the preparation of external skin ointments or cosmetics is 0.0001-10.0% by weight, preferably 0.0005-10.0% by weight in dry weight. A clear effect could not be expected at concentrations below 0.0001% by weight, and no increase in effect was seen at concentrations above 10% by weight.

다음으로 실시예에 의거하여 본 발명을 자세히 설명하고자 하며, 본 발명이 실시예에만 한정되는 것이 아님을 밝혀둔다.
Next, the present invention will be described in detail with reference to Examples, and the present invention is not limited only to Examples.

실시예 1-12Example 1-12

시판되는 로로통, 백미를 구입하여 분쇄한 분쇄물 100g을 물이나, 탄소수 1-4개의 무수 또는 함수 저급알코올, 에틸아세테이트 또는 아세톤등의 용매 3L에 넣고, 냉각콘덴서가 달린 환류 추출기에서 3시간 끓여 추출한 다음, 100메쉬 여과포로 여과한 후 잔사를 같은 방법으로 1회 더 추출하였다. 각각의 추출액을 합하여 상온에서 화트만(Whatman) 2번 여과지로 여과하여 불용성물질을 제거한 후, 냉각 콘덴서가 달린 증류장치에서 60oC로 감압농축한 후 동결건조하여 표1과 같이 각각의 건조 중량을 얻었다. Purchasing commercially available Roroton and white rice, 100 g of pulverized powder is placed in 3 L of solvent such as water, anhydrous or hydrous lower alcohol having 1 to 4 carbon atoms, ethyl acetate or acetone, and boiled for 3 hours in a reflux extractor with a cooling capacitor. After extraction, the resultant was filtered with 100 mesh filter cloth and the residue was extracted once more in the same manner. Each extract was combined and filtered using Whatman No. 2 filter paper at room temperature to remove insoluble materials, concentrated under reduced pressure at 60 o C in a distillation apparatus equipped with a cooling condenser, and lyophilized to dry weight as shown in Table 1 below. Got.

추출용매 및 추출물의 건조중량Dry weight of extractant and extract 로로통Roroton 백미White rice 80%메탄올80% Methanol 7.5g(실시예1)7.5 g (Example 1) 9.8g(실시예7)9.8 g (Example 7) 정제수Purified water 6.8g(실시예2)6.8 g (Example 2) 8.2g(실시예8)8.2g (Example 8) 85%에탄올85% Ethanol 8.0g(실시예3)8.0g (Example 3) 9.3g(실시예9)9.3 g (Example 9) 70%아세톤70% Acetone 6.9g(실시예4)6.9 g (Example 4) 7.3g(실시예10)7.3 g (Example 10) 에칠아세테이트Ethyl Acetate 6.3g(실시예5)6.3 g (Example 5) 7.2g(실시예11)7.2 g (Example 11) 포화노말부탄올Saturated normal butanol 7.7g(실시예6)7.7g (Example 6) 8.6g(실시예12)8.6 g (Example 12)

실험예 1Experimental Example 1

상기 실시예 1-12에 따라 얻어진 각 추출물들을 쥐의 멜라노마 세포(B-16 mouse melanoma cell)의 배양액에 첨가하여 세포수준에서의 미백 효과를 실험하였다.(Lotan R., Lotan D. Cancer Res. 40:3345-3350, 1980). 실시예 1-12에 따라 얻어진 각 추출물들을 최종농도가 0.005 %가 되도록 하여 하이드로퀴논 수용액과 함께 각각 B-16멜라노마 세포의 배양배지에 첨가하여 3일간 배양한 후 세포들을 트립신(trypsin)처리하여 배양용기로 부터 떼어내 원심분리한 후 멜라닌을 추출하였다. 이것에 수산화 나트륨 용액(1N농도) 1ml를 가하여 10분간 끓여 멜라닌을 녹이 고 분광 광도계를 이용, 400나노미터(nm)에서 흡광도를 측정하여 생성된 멜라닌의 양을 단위 세포수당(106 cell)의 흡광도로 나타내는 방법으로 수행하였으며, 대조군에 대한 상대적인 멜라닌 생성량을 저해율(%)로 계산하고 결과를 표 2에 정리하였다. Each of the extracts obtained according to Examples 1-12 was added to the culture medium of B-16 mouse melanoma cells to test the whitening effect at the cellular level. (Lotan R., Lotan D. Cancer Res 40: 3345-3350, 1980). Each extract obtained according to Example 1-12 was added to a culture medium of B-16 melanoma cells with an aqueous hydroquinone solution and then cultured for 3 days with a final concentration of 0.005%, followed by trypsin treatment. Melanin was extracted from the culture vessel by centrifugation. To this was added sodium hydroxide solution (1N concentration) 1ml hydroxide rusted melanin boiled 10 minutes using a spectrophotometer at 400 nanometers (nm) The amount of the unit cell allowance (10 6 cell) of melanogenesis by measuring the absorbance at It was carried out by the method represented by the absorbance, the relative melanin production relative to the control was calculated as the inhibition rate (%) and the results are summarized in Table 2.

하기 표 2의 결과에서 볼 수 있듯이, 실시예 1-12에 따라 얻어진 각 시료들은 전혀 정제되지 않은 추출물임을 감안하면 기존에 알려진 미백물질인 하이드로퀴논과 비교할 때 배양된 쥐의 멜라노마 세포에 대하여 매우 강력한 멜라닌 생성 억제능이 있음을 알 수 있다.As can be seen from the results in Table 2, considering that each sample obtained according to Examples 1-12 is an extract that is not purified at all, compared to the hydroquinone which is a known whitening substance, it is very good for the melanoma cells of cultured mice. It can be seen that there is a strong melanin production inhibitory ability.

로로통, 백미 추출물의 세포수준에서의 멜라닌 생성 저해효과Inhibitory Effects of Roroton and White Rice Extracts on the Cell Level of Melanin Production 시료sample 멜라닌 생성Melanin production 저해율(%)% Inhibition 대조군(무첨가)Control group (no addition) 0.048±0.0030.048 ± 0.003 -- 실시예 1(최종농도 0.005%)Example 1 (final concentration 0.005%) 0.030±0.0030.030 ± 0.003 38%38% 실시예 2(최종농도 0.005%)Example 2 (final concentration 0.005%) 0.033±0.0030.033 ± 0.003 31%31% 실시예 3(최종농도 0.005%)Example 3 (final concentration 0.005%) 0.028±0.0020.028 ± 0.002 42%42% 실시예 4(최종농도 0.005%)Example 4 (final concentration 0.005%) 0.026±0.0020.026 ± 0.002 46%46% 실시예 5(최종농도 0.005%)Example 5 (final concentration 0.005%) 0.023±0.0030.023 ± 0.003 53%53% 실시예 6(최종농도 0.005%)Example 6 (final concentration 0.005%) 0.030±0.0030.030 ± 0.003 38%38% 실시예 7(최종농도 0.005%)Example 7 (final concentration 0.005%) 0.034±0.0040.034 ± 0.004 29%29% 실시예 8(최종농도 0.005%)Example 8 (final concentration 0.005%) 0.036±0.0020.036 ± 0.002 25%25% 실시예 9(최종농도 0.005%)Example 9 (final concentration 0.005%) 0.033±0.0020.033 ± 0.002 31%31% 실시예10(최종농도 0.005%)Example 10 (final concentration 0.005%) 0.027±0.0020.027 ± 0.002 44%44% 실시예11(최종농도 0.005%)Example 11 (final concentration 0.005%) 0.025±0.0020.025 ± 0.002 48%48% 실시예12(최종농도 0.005%)Example 12 (final concentration 0.005%) 0.022±0.0020.022 ± 0.002 54%54% 하이드로퀴논 (최종농도0.0001% )     Hydroquinone (final concentration 0.0001%) 0.025±0.0020.025 ± 0.002 48%48%

* 반복수 = 3                                                           * Number of iterations = 3

실험예 2Experimental Example 2

실험예 1과 같은 방법으로 배양된 쥐의 멜라노마 세포에 대하여 실시예1, 7 의 추출물에 대하여 농도에 따른 멜라닌 생성 억제능을 조사하였으며 결과는 표 3과 같다.Melamine production of rats cultured in the same manner as in Experimental Example 1 was investigated for the melanin production inhibitory ability according to the concentration of the extract of Examples 1, 7 and the results are shown in Table 3.

농도에 따른 세포수준에서의 멜라닌 생성 저해효과Inhibitory effect of melanin production at the cellular level 시료sample 적용농도(%)Application concentration (%) 멜라닌생성량Melanin production 저해율(%)% Inhibition 대조군(무첨가)Control group (no addition) -- 0.048±0.0040.048 ± 0.004 -- 실시예 1Example 1 최종농도(0.0005 %)Final concentration (0.0005%) 0.040±0.0020.040 ± 0.002 17%17% 최종농도(0.005%)Final concentration (0.005%) 0.030±0.0030.030 ± 0.003 38%38% 최종농도(0.05 %)Final concentration (0.05%) 0.026±0.0020.026 ± 0.002 46%46% 최종농도(0.5%)Final concentration (0.5%) 0.022±0.0010.022 ± 0.001 54%54% 실시예 7Example 7 최종농도(0.0005 %)Final concentration (0.0005%) 0.041±0.0020.041 ± 0.002 7%7% 최종농도(0.005%)Final concentration (0.005%) 0.034±0.0040.034 ± 0.004 29%29% 최종농도(0.05 %)Final concentration (0.05%) 0.028±0.0020.028 ± 0.002 42%42% 최종농도(0.5%)Final concentration (0.5%) 0.022±0.0010.022 ± 0.001 54%54% 하이드로퀴논Hydroquinone (0.0001%)(0.0001%) 0.025±0.0020.025 ± 0.002 48%48%

●반복수=3Repeat number = 3

상기 표 3의 결과에서 볼 수 있듯이, 로로통, 백미 추출물은 배양된 쥐의 멜라노마 세포에 대하여 매우 강력한 멜라닌 생성 억제능을 가지고 있음을 알 수 있다. 하이드로퀴논은 저농도에서 강력한 멜라닌 생성 억제능을 가지지만 세포 독성이 심해 0.0001%이상에서는 실험을 할 수 없는 것에 반하여, 본 발명에서의 추출물들은 0.05%농도 이상에서도 세포독성을 나타내지 않으면서 사용가능한 최대량의 하이드로퀴논보다 높은 멜라닌 생성 억제 효과를 갖는다. 또한 로로통, 백미 추출물이 단일물질이 아니고 혼합물질이라는 것을 고려할 때 매우 높은 멜라닌 생성 억제능을 가지고 있으므로, 기미나 주근깨 개선 또는 피부미백에 매우 유용하게 사용될 수 있다.As can be seen in the results of Table 3, Roroton, white rice extract can be seen that it has a very strong melanin production inhibitory ability against cultured melanoma cells. Hydroquinone has a strong melanin production inhibitory ability at low concentrations, but the cytotoxicity is severe and can not be experimented at 0.0001% or more, whereas the extract of the present invention is the maximum amount of hydro that can be used without showing cytotoxicity at 0.05% or more concentration It has a higher melanin production inhibitory effect than quinone. In addition, Roroton, white rice extract has a very high melanin production inhibitory ability, considering that it is not a single substance but a mixture, it can be very useful for improving skin or freckles or skin whitening.

이하, 로로통, 백미 추출물을 함유하는 화장료의 처방예를 제조예에 의해 나타내었다. Hereinafter, the formulation example of the cosmetics containing Roroton and white rice extract was shown by the manufacture example.                     

제조예 1-2 및 비교예 1Preparation Example 1-2 and Comparative Example 1

로로통, 백미 추출물을 함유하는 피부 외용연고 처방예는 다음과 같다.An example of external skin ointment containing Roroton and white rice extract is as follows.

여기서, 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.Here, Roroton and white rice extracts refer to those of Examples 5 and 11, respectively.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 1One 22 1One -추 출 물 로로통 추출물 백미 추출물 -디에틸 세바케이트 -경납 -폴리옥시에틸렌올레일에테르 포스페이트 -벤조산 나트륨 -바셀린-Extract Roroton Extract White Rice Extract                                               -Diethyl Sebacate-Brazing-Polyoxyethylene Oleyl Ether Phosphate-Sodium Benzoate-Vaseline 10 - 8 5 6 적량 to 100 10-8 5 6 Suitable to 100 - 10 8 5 6 적량 to 100 -10 8 5 6 Suitable to 100 - - 8 5 6 적량 to 100 --8 5 6 Suitable to 100

제조예 3-4및 비교예 2Preparation Example 3-4 and Comparative Example 2

로로통, 백미 추출물을 함유하는 화장료 중 크림의 처방예는 다음과 같다. 여기서 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.
A prescription example of a cream in cosmetics containing Roroton and white rice extract is as follows. Roroton and white rice extracts here refer to those of Examples 5 and 11.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 33 44 22 -추 출 물 로로통 추출물 백미 추출물 - 스테아린산 -세탄올 -수산화칼륨 -글리세린 -프로필렌글리콜 -방부제 -향 -정제수-Extract Roroton Extract White Rice Extract                                              -Stearic acid-Cetanol-Potassium hydroxide-Glycerine-Propylene glycol-Preservative-Fragrance-Purified water 1.0 - 15.0 1.0 0.7 5.0 3.0 적량 적량 to 100 1.0-15.0 1.0 0.7 5.0 3.0 Proper quantity to 100 - 1.0 15.0 1.0 0.7 5.0 3.0 적량 적량 to 100  -1.0 15.0 1.0 0.7 5.0 3.0 Proper amount to 100 - - 15.0 1.0 0.7 5.0 3.0 적량 적량 to 100 --15.0 1.0 0.7 5.0 3.0 Proper quantity to 100

제조예 5-6 및 비교예 3Preparation Example 5-6 and Comparative Example 3

로로통, 백미 추출물을 함유하는 화장료 중 유연화장수의 처방예는 다음과 같다. 여기서 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.Roroton, a prescription example of the softening of the cosmetics containing white rice extract is as follows. Roroton and white rice extracts here refer to those of Examples 5 and 11.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 55 66 22 -추 출 물 로로통 추출물 백미 추출물 - 에탄올 -폴리라우린산폴리옥시에틸렌소르 비탄 -파라옥시안식향산메칠 -글리세린 -1,3-부틸렌글리콜 -향 -색소 -정제수-Extract Roroton Extract White Rice Extract                                              -Ethanol-Polylauric acid Polyoxyethylene sorbent Non-Paraoxybenzoic acid methyl-Glycerin-1,3-butylene glycol-Flavor-Pigment-Purified water 0.2 - 10.0 1.0 0.2 5.0 6.0 적량 적량 to 100 0.2-10.0 1.0 0.2 5.0 6.0 Proper volume to 100 - 0.2 10.0 1.0 0.2 5.0 6.0 적량 적량 to 100 -0.2 10.0 1.0 0.2 5.0 6.0 Proper amount to 100 - - 10.0 1.0 0.2 5.0 6.0 적량 적량 to 100 --10.0 1.0 0.2 5.0 6.0 Proper amount to 100

제조예 7-8 및 비교예 4Preparation Example 7-8 and Comparative Example 4

로로통, 백미 추출물 함유하는 화장료 중 영양화장수의 처방예는 다음과 같다. 여기서 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.Roroton, a white rice extract containing a cosmetic example of nutritional longevity is as follows. Roroton and white rice extracts here refer to those of Examples 5 and 11.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 77 88 44 -추 출 물 로로통 추출물 백미 추출물 -바셀린 -세스퀴올레인산소르비탄 -폴리옥시에틸렌올레일에틸 -파라옥시안식향산메칠 -프로필렌글리콜 -에탄올 -카르복시비닐폴리머 -수산환칼륨 -색소 -향 -정제수-Extract Roroton Extract White Rice Extract                                              -Vaseline-Sesquioleate sorbitan-Polyoxyethylene oleyl ethyl-Paraoxybenzoic acid methyl-Propylene glycol-Ethanol-Carboxy vinyl polymer-Potassium oxalate-Pigment-Flavor-Purified water 0.1 - 2.0 0.8 1.2 적량 5.0 3.2 18.0 0.1 적량 적량 to 100 0.1-2.0 0.8 1.2 appropriate 5.0 3.2 18.0 0.1 appropriate volume to 100 - 0.1 2.0 0.8 1.2 적량 5.0 3.2 18.0 0.1 적량 적량 to 100 -0.1 2.0 0.8 1.2 Accurate 5.0 3.2 18.0 0.1 Accurate to 100 - - 2.0 0.8 1.2 적량 5.0 3.2 18.0 0.1 적량 적량 to 100 --2.0 0.8 1.2 Suitable 5.0 3.2 18.0 0.1 Suitable to 100

제조예 9-10 및 비교예 5Preparation Example 9-10 and Comparative Example 5

로로통, 백미 추출물을 함유하는 화장료 중 팩의 처방예는 다음과 같다. 여 기서 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.Prescription of the pack of cosmetics containing Roroton, white rice extract is as follows. Here Rorotong, white rice extract refers to those of Examples 5 and 11, respectively.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 99 1010 55 -추 출 물 로로통 추출물 백미 추출물 - 글리세린 -프로필렌글리콜 -폴리비닐알코올 -에탄올 -폴리옥시에틸렌올레일에칠 -파라옥시안식향산메칠 -향 -색소 -정제수-Extract Roroton Extract White Rice Extract                                              -Glycerine-Propylene glycol-Polyvinyl alcohol-Ethanol-Polyoxyethylene oleyl ethyl-Paraoxybenzoic acid methyl-Flavor-Pigment-Purified water 0.5 - 5.0 4.0 15.0 8.0 1.0 0.2 적량 적량 to 100 0.5-5.0 4.0 15.0 8.0 1.0 0.2 Proper volume to 100 - 0.5 5.0 4.0 15.0 8.0 1.0 0.2 적량 적량 to 100 -0.5 5.0 4.0 15.0 8.0 1.0 0.2 Correct Volume to 100 - - 5.0 4.0 15.0 8.0 1.0 0.2 적량 적량 to 100 --5.0 4.0 15.0 8.0 1.0 0.2 Proper titration to 100

제조예 11-12 및 비교예 6Preparation Example 11-12 and Comparative Example 6

로로통, 백미 추출물을 함유하는 화장료 중 에셋스의 처방예는 다음과 같다. 여기서 로로통, 백미 추출물은 각각 실시예 5, 11의 것을 말한다.Roroton, a prescription example of the assets in the cosmetics containing white rice extract is as follows. Roroton and white rice extracts here refer to those of Examples 5 and 11.

조성물Composition 제조예(중량%)Production example (% by weight) 비교예Comparative example 1111 1212 66 -추 출 물 로로통 추출물 백미 추출물 -프로필렌글리콜 -글리세린 -히아루론산나트륨수용액(1%) -에탄올 -폴리옥시에틸렌경화피마자유 -파라옥시안식향산메칠 -향 -정제수-Extract Roroton Extract White Rice Extract                                              -Propylene glycol-Glycerine-Sodium hyaluronate aqueous solution (1%)-Ethanol-Polyoxyethylene hardened castor oil-Paraoxybenzoic acid methyl-Flavor-Purified water 5 - 10.0 10.0 5.0 5.0 1.0 0.1 적량 to 100 5-10.0 10.0 5.0 5.0 1.0 0.1 dose to 100 - 5 10.0 10.0 5.0 5.0 1.0 0.1 적량 to 100 -5 10.0 10.0 5.0 5.0 1.0 0.1 dose to 100 - - 10.0 10.0 5.0 5.0 1.0 0.1 적량 to 100 --10.0 10.0 5.0 5.0 1.0 0.1 dose to 100

실험예 3Experimental Example 3

건강한 남여 20명씩을 선정하여 양팔의 하박부에 직경 7mm크기의 구멍이 6개 씩 2줄로 파인 알루미늄 호일을 붙이고, 팔에서 10cm 떨어진 거리에서 ORIEL solar simulator 1000W를 사용하여 60mJ/cm2의 광량을 조사하였다. 조사전에 70% 에탄올 수용액으로 조사부위를 잘 세척하였다. 조사하기 3일전부터 조사 후 3주째까지 1일 2회씩 제조예 1-12및 비교예 1-6에 따라 제조된 로로통, 백미 추출물을 함유한 시료와 각각의 추출물이 함유되지 않은 기제를 한 쌍으로 같은 줄에 도포하였다.(제조예 9, 10, 및 비교예 5의 팩 처방의 경우 도포한 다음 15분 후에 떼어내었다.) 각각에 대하여 제조예와 비교예의 색소침착도를 육안으로 판정하고, 제조예가 비교예에 비해 색소침착을 억제한 정도를 뚜렷한 효과, 효과있음, 차이없음의 3단계로 평가하였으며, 그 결과는 표 4과 같다.Select 20 healthy males and females, and attach the aluminum foil with 6 holes of 7mm diameter in two rows to the lower forearm of each arm and irradiate 60mJ / cm 2 light using ORIEL solar simulator 1000W at a distance of 10cm from the arm. It was. The irradiation site was washed well with 70% ethanol aqueous solution before irradiation. A pair of Roroton, a sample containing white rice extract prepared in accordance with Preparation Examples 1-12 and Comparative Examples 1-6, and a base not containing each extract, twice a day from 3 days before irradiation to 3 weeks after irradiation. (In the case of the pack formulations of Preparation Examples 9, 10, and Comparative Example 5, the coating was removed 15 minutes after application.) For each, the pigmentation degree of Preparation Example and Comparative Example was visually determined. Preparation Example evaluated the degree of inhibiting the pigmentation compared to the comparative example in three steps of distinct effects, effects, no difference, the results are shown in Table 4.

로로통, 백미 추출물을 함유한 연고 및 화장료의 색소 침착 저해 효과Inhibition of Pigmentation of Ointments and Cosmetics Containing Roroton and White Rice Extracts 실험물질 Experimental substance 뚜렷한 효과(명)Distinct Effects (persons) 효과있음(명)Effective (persons) 차이없음(명)No difference (persons) 제조예 1Preparation Example 1 44 88 88 제조예 2Preparation Example 2 44 99 77 제조예 3Preparation Example 3 33 88 99 제조예 4Preparation Example 4 33 77 1010 제조예 5Preparation Example 5 22 99 88 제조예 6Preparation Example 6 22 88 1010 제조예 7Preparation Example 7 22 88 1010 제조예 8Preparation Example 8 22 99 99 제조예 9Preparation Example 9 22 1010 88 제조예 10Preparation Example 10 33 88 99 제조예 11Preparation Example 11 33 88 99 제조예 12Preparation Example 12 33 99 88

상기 표 4의 결과에서 볼 수 있듯이, 제조예 1-12에 따라 제조된 로로통, 백미 추출물이 함유된 미백연고 및 화장료는 피시험자 20명 중에서 최소 10명 이상에 대하여 미백 효과를 나타내었으며, 특히 많은 양의 로로통, 백미 추출물이 적용된 제조예 1, 2와 비교예1의 비교 실험에서는 60%가 색소 침착 저해 효과를 보이고, 피부내에서 어떤 부작용도 나타나지 않아, 로로통, 백미 추출물이 안전하고 효과가 매우 뛰어난 기미나 주근깨 개선 또는 피부미백용 화장료 임을 알 수 있다.As can be seen from the results of Table 4, the Roroton, the whitening ointment and the cosmetic containing the white rice extract prepared according to Preparation Example 1-12 showed a whitening effect on at least 10 or more of 20 subjects, in particular In the comparative experiments of Preparation Examples 1 and 2 and Comparative Example 1 to which a large amount of Roroton and White rice extract were applied, 60% showed pigmentation inhibitory effect, and no side effects appeared in the skin. It can be seen that it is very effective in improving the appearance of freckles or skin whitening.

이상 설명하고 실시예와 비교예를 통하여 알 수 있는 바와 같이, 본 발명의 로로통, 백미 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 화장료 조성물은 미백 효과 및 색소 침착 저해 효과를 보이며 피부내에서 어떤 부작용도 나타나지 않아 안전하고 기미나 주근깨 개선효과가 우수하다.











As described above and can be seen through the Examples and Comparative Examples, the cosmetic composition containing at least one selected from Roroton, white rice extract of the present invention as an active ingredient shows a whitening effect and pigmentation inhibitory effect in the skin Does not show any side effects and is safe and improves freckles and freckles.











Claims (3)

로로통 추출물 및 백미(Cynanchum atratum Bunge.) 추출물에서 선택되는 1종 이상을 유효성분으로 함유하는 것을 특징으로 하는 기미, 주근깨 개선 및 피부 미백효과를 나타내는 화장료 조성물.A cosmetic composition exhibiting blemishes, freckles, and skin whitening effects, comprising at least one selected from Roroton extract and Cynanchum atratum Bunge. Extract as an active ingredient. 제 1 항에 있어서, 로로통 추출물 및 백미(Cynanchum atratum Bunge.) 추출물에서 선택되는 1종 이상을 각각 건조 중량으로 0.0001 내지 10.0 중량% 함유하는 것을 특징으로 하는 화장료 조성물.The cosmetic composition according to claim 1, which contains 0.0001 to 10.0% by weight of at least one selected from Roroton extract and Cynanchum atratum Bunge. Extract, respectively, in dry weight. 제 1 항에 있어서, 로로통 추출물 및 백미(Cynanchum atratum Bunge.) 추출물은 각각 물, 탄소수 1 내지 4의 저급 알코올, 에틸아세테이트 또는 아세톤으로 1회 이상 추출하고, 추출액을 감압 증류한 후 동결 건조하거나 분사 건조하여 얻은 추출물인 것을 특징으로 하는 화장료 조성물.According to claim 1, Rorotong extract and Cynanchum atratum Bunge. Extract is extracted one or more times with water, lower alcohol having 1 to 4 carbon atoms, ethyl acetate or acetone, respectively, the extract is distilled under reduced pressure and freeze-dried Cosmetic composition, characterized in that the extract obtained by spray drying.
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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR101047588B1 (en) * 2008-07-29 2011-07-08 충북대학교 산학협력단 Whitening composition comprising white rice extract and novel pregnan compound isolated therefrom as active ingredient
CN102329358A (en) * 2011-05-31 2012-01-25 苏州派腾生物医药科技有限公司 Preparation method of cynatratoside A
KR101823928B1 (en) 2016-05-31 2018-01-31 주식회사 아이썸 Composition for skin whitening comprising extract of Cynanchum ascyrifolium as effective component
KR20210024730A (en) * 2019-08-26 2021-03-08 주식회사 테트라코스메틱 Compositon comprising fermented product of Cynanchi atrati Radix as an active ingredient for skin whitening

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP5117092B2 (en) * 2007-04-09 2013-01-09 株式会社ノエビア Moisturizer, anti-aging agent, whitening agent, antioxidant, slimming agent, treatment agent, arginase activity promoter and external preparation for skin
KR101768870B1 (en) * 2015-04-13 2017-08-17 주식회사 래디안 Cosmetic composition and pharmaceutical composition with sinapic acid or the extract of cynanchum atratum for wound healing

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR920005683A (en) * 1990-04-12 1992-04-03 원본미기재 Herbicidal composition having a synergistic effect
KR920005683B1 (en) * 1987-10-12 1992-07-13 서영유 Soap composition from plants
JPH08268837A (en) * 1995-03-31 1996-10-15 Lion Corp Emulsion-type composition

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR920005683B1 (en) * 1987-10-12 1992-07-13 서영유 Soap composition from plants
KR920005683A (en) * 1990-04-12 1992-04-03 원본미기재 Herbicidal composition having a synergistic effect
JPH08268837A (en) * 1995-03-31 1996-10-15 Lion Corp Emulsion-type composition

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR101047588B1 (en) * 2008-07-29 2011-07-08 충북대학교 산학협력단 Whitening composition comprising white rice extract and novel pregnan compound isolated therefrom as active ingredient
CN102329358A (en) * 2011-05-31 2012-01-25 苏州派腾生物医药科技有限公司 Preparation method of cynatratoside A
KR101823928B1 (en) 2016-05-31 2018-01-31 주식회사 아이썸 Composition for skin whitening comprising extract of Cynanchum ascyrifolium as effective component
KR20210024730A (en) * 2019-08-26 2021-03-08 주식회사 테트라코스메틱 Compositon comprising fermented product of Cynanchi atrati Radix as an active ingredient for skin whitening
KR102226346B1 (en) 2019-08-26 2021-03-11 주식회사 테트라코스메틱 Compositon comprising fermented product of Cynanchi atrati Radix as an active ingredient for skin whitening

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