KR100955298B1 - Fermented Extract Preparation Method of Eoseongcho and Sambaekcho - Google Patents
Fermented Extract Preparation Method of Eoseongcho and Sambaekcho Download PDFInfo
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- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K36/00—Medicinal preparations of undetermined constitution containing material from algae, lichens, fungi or plants, or derivatives thereof, e.g. traditional herbal medicines
- A61K36/18—Magnoliophyta (angiosperms)
- A61K36/185—Magnoliopsida (dicotyledons)
- A61K36/78—Saururaceae (Lizard's-tail family)
-
- A—HUMAN NECESSITIES
- A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
- A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
- A61K2236/00—Isolation or extraction methods of medicinal preparations of undetermined constitution containing material from algae, lichens, fungi or plants, or derivatives thereof, e.g. traditional herbal medicine
- A61K2236/30—Extraction of the material
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- Biotechnology (AREA)
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- Pharmacology & Pharmacy (AREA)
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Abstract
본 발명은 어성초와 삼백초의 발효추출물 제조방법에 관한 것으로서, 보다 상세하게는 어성초 또는 삼백초를 발효시켜 숙성한 후 열수 및 에탄올 추출하여 어성초 또는 삼백초의 발효추출물을 제조하는 방법에 관한 것이다.The present invention relates to a method for producing fermented extract of Eochocho and three hundred gree, and more particularly to fermented extract of Eochocho or three hundred gree after fermentation of Echochocho or three hundred vine, followed by hot water and ethanol extraction.
본 발명에 따른 발효추출물 제조방법은 어성초 및 삼백초의 비린 맛과 향이 제거되면서, 어성초와 삼백초에 함유된 유용성분들을 약리효과의 감소 없이 추출하는 방법을 제공한다.Fermentation extract manufacturing method according to the present invention, while removing the fishy taste and aroma of eoseongcho and three hundred seconds, provides a method for extracting the useful ingredients contained in eoseongcho and three hundred seconds without reducing the pharmacological effect.
Description
본 발명은 어성초 또는 삼백초를 발효시켜 숙성한 후 열수 및 에탄올 추출하여 어성초 또는 삼백초의 발효추출물을 제조하는 방법에 관한 것이다.The present invention relates to a method for producing fermented extract of Eochocho or three hundred sec by fermenting Eochocho or three hundred sec, followed by hot water and ethanol extraction.
최근, 생활패턴의 변화로 인한 운동부족, 과로, 스트레스, 질병 및 체질악화 등을 해소하기 위한 기능성을 갖는 자연 건강식품에 대한 수요가 급격히 증가하고 있으며, 그에 대한 연구개발이 활발히 진행되고 있다.Recently, the demand for a natural health food having a function to solve the lack of exercise, overwork, stress, disease and constitution due to changes in lifestyle patterns is rapidly increasing, and the research and development is actively progressed.
그 일환으로서, 이뇨작용, 진통작용, 지혈작용, 항균작용, 항바이러스작용, 항혈관확장작용 및 소염작용 등에 약효가 좋은 어성초(Houttuynia cordata Thunb.)와, 항균, 해열, 해독, 소염, 간염, 황달, 종기, 화농, 살충, 상처, 궤양치료, 발암성 물질의 활성감소, 암세포의 생육저해 및 혈압강화 등에 약효가 좋은 삼백초(saururus chinensis Baill.)에 대한 연구가 진행중에 있다.As part of this, Houttuynia cordata Thunb., Which is effective in diuretic, analgesic, hemostatic, antimicrobial, antiviral, anti-angiogenic and anti-inflammatory effects, antibacterial, antipyretic, detoxifying, anti-inflammatory, hepatitis, Research is underway on saururus chinensis Baill., Which is effective for jaundice, boils, purulent insecticides, wounds, ulcers, deactivation of carcinogenic substances, inhibiting cancer cell growth and strengthening blood pressure.
어성초는 삼백초과에 속하는 다년생 초본의 야생약초로서 주요 성분으로는 테르페노이드(terpenoid), 지질(lipid) 및 방향족 계통의 휘발성 성분과 퀘세 틴(quercetin), quercetin-3-o-glycoside 계통의 후라보노이드 화합물로 알려져 있으며 예로부터 생약재로 널리 이용되어 왔다. 또한, 삼백초는 중국, 일본을 비롯해 우리나라에서는 북제주군 한경면 고습지와 바닷가에서 주로 자생하는 다년초로서, 주요 성분으로서 퀘세틴(quercetin)과 쿼시트린(quercitrin)을 함유하고 있는 건강식품 재료 중의 하나이다.Eoseongcho is a wild herb of perennial herb that belongs to over three hundred species. Its main components are terpenoid, lipid and aromatic volatile components, quercetin and quercetin-3-o-glycoside. It is known as and has been widely used as a herbal medicine since ancient times. In addition, the three hundred vinegar is a perennial herb that grows mainly in the high wetlands and beaches of Hankyung-myeon, Bukjeju-gun in China, Japan, and Korea.
상기와 같은 어성초와 삼백초는 각각 함유하고 있는 성분 때문에 생선 비린내와 같은 강하고 독특한 냄새를 발산하게 된다. 상기와 같은 어성초와 삼백초에서 발산하는 비린내를 제거하기 위해, 종래에는 어성초와 삼백초를 건조하거나 수증기를 통해 증류시켜 약제로 가공하는 이용하는 방법을 사용하고 있다. 그러나, 상기와 같은 종래의 방법은 어성초와 삼백초가 갖는 비린 냄새를 완전히 제거하지 못하기 때문에, 비위가 약한 복용자가 생식하는데 거부감을 주는 문제점이 있다.Echoseong and three hundred seconds as described above because of the components that each contain a strong and unique smell, such as fish fishy. In order to remove fishy odor from the above-mentioned Echo and three hundred seconds, conventionally, Echo and three hundred seconds to dry or distilled through the water vapor is used to process the drug. However, since the conventional method as described above does not completely remove the fishy smell of fish and 300 seconds, the weaker nausea has a problem of rejection for reproduction.
또한, 상기와 같은 종래의 방법은 건조 및 수증기를 통해 증류시켜서 약제로 가공하는 과정에서 어성초와 삼백초 특유의 약리효과를 감소시키는 문제점이 있다.In addition, the conventional method as described above has a problem of reducing the pharmacological effects peculiar to Eochocho and three hundred sec in the process of drying and distilling through water vapor into a drug.
이에, 본 발명자들은 어성초, 삼백초가 가지고 있는 기능성을 향상시킨 발효액제조기술을 연구하던 중, 어성초 및 삼백초의 건체 열수추출액 및 발효숙성액의 효율적 제조기술을 개발하고, 이로부터 유용물질들을 추출하는 방법을 확립함으로써 본 발명을 완성하였다.Therefore, the inventors of the present invention while studying the fermentation broth production technology to improve the functionality of Eoseongcho, three hundred seconds, develop efficient manufacturing technology of dry hot water extract and fermentation matured liquid of Eoseongcho and three hundred seconds, the method of extracting useful substances therefrom The present invention has been completed by establishing.
본 발명의 목적은 어성초 및 삼백초의 발효추출물을 제조하는 방법을 제공하는 것이다.It is an object of the present invention to provide a method for preparing fermented extracts of fishery herb and three hundred herb.
상기 목적을 달성하기 위하여, 본 발명은 어성초 또는 삼백초를 세척한 후 물기를 제거하는 단계; 상기 물기가 제거된 어성초 또는 삼백초를 항아리에 넣고 그 위에 설탕시럽을 첨가하고, 상기 어성초 또는 삼백초에 설탕시럽을 첨가하는 작업을 반복시행하여 적층하는 단계; 상기 적층된 상부 표면의 어성초 또는 삼백초가 완전히 덮이도록 설탕시럽을 도포하는 단계; 상기 설탕시럽이 도포된 상부 표면을 깨끗한 돌로 눌러두는 단계; 상기 항아리를 밀봉시킨 후 1차 발효를 수행하는 단계; 상기 1차 발효물의 생성된 거품을 안정화시키고 2차 발효를 수행하는 단계; 상기 2차 발효물을 상온에서 2~3개월간 숙성 및 침출한 후 여과하여 발효숙성액을 제조하는 단계; 상기 발효숙성액에 중량기준 10배의 증류수를 가한 다음 95℃에서 8시간 열수 추출하고 여과하여 여과액을 제조하는 단계; 상기 여과액을 상기 증류수 기준 5부피%가 되도록 50~55℃에서 감압농축한 후 상온으로 냉각하여 농축액을 제조하는 단계; 상기 농축액에 75% 에탄올을 가하여 교반하고 5℃에서 24시간 방치하는 단계; 및 상기 방치된 농축액을 여과한 후 동결건조하여 분말로 제조하는 단계를 포함하는, 어성초와 삼백초의 발효추출물 제조방법을 제공한다.In order to achieve the above object, the present invention comprises the steps of removing the water after washing Eoseongcho or three hundred seconds; Putting the water-removed fish vinegar or three hundred vine into a jar and adding sugar syrup to the jar, and repeating the operation of adding sugar syrup to the fish vinegar or three hundred s; Applying a sugar syrup to completely cover the fish paste or three hundred candles of the laminated upper surface; Pressing the sugar syrup-coated upper surface with a clean stone; Sealing the jar and performing primary fermentation; Stabilizing the resulting foam of the primary fermentation and performing secondary fermentation; Aging and leaching the secondary fermented product at room temperature for 2 to 3 months and then filtering to prepare a fermented matured liquid; Adding distilled water 10 times by weight to the fermentation broth, followed by extracting hot water at 95 ° C. for 8 hours and filtering to prepare a filtrate; Preparing a concentrated solution by concentrating the filtrate under reduced pressure at 50˜55 ° C. such that the filtrate is 5 vol% based on the distilled water; 75% ethanol was added to the concentrate, followed by stirring for 24 hours at 5 ° C; And it provides a method for producing a fermented extract of Eoseongcho and three hundred seconds, comprising the step of filtering the left concentrate and lyophilized to produce a powder.
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본 발명자들은 어성초와 삼백초 각각의 시료로부터 발효추출물을 제조하였다. 먼저, 설탕시럽과 어성초 또는 삼백초를 혼합하여 1차 발효 및 2차 발효를 수행한 후, 상온에서 숙성 및 침출하여 발효숙성액을 제조하였다. 또한, 어성초 및 삼백초 각각에 대한 열수 및 알코올 추출을 수행하였다(도 1 참조).The present inventors prepared fermented extracts from the samples of Eoseongcho and three hundred sec. First, the sugar syrup and Eoseongcho or three hundred vines were mixed to carry out the first fermentation and the second fermentation, and then aged and leached at room temperature to prepare a fermentation matured liquid. In addition, hydrothermal and alcohol extraction was carried out for each of the fish and 300 seconds (see Fig. 1).
아울러, 어성초 및 삼백초 각각의 성분을 메탄올을 이용한 추출 후에 일반성분을 분석하였다(표 1 참조). 일반성분의 경우 어성초, 삼백초 공히 다른 성분에 비해 높은 함량을 나타내었으며 총비타민C 함량은 다른 약초류에 비해 높은 함량을 나타내었다. 또한, 어성초 및 삼백초의 유리당 함량을 측정한 결과, 다른 녹차잎에 비해서는 과당과 포도당 함량은 비교적 높은 편이었으며 설탕과 말토스 함량은 녹차잎, 감잎에 비해 비슷하거나 그보다 낮다(표 2 참조). 또한, 어성초 및 삼백초 각각 발효추출액의 Bacillus속 균주에 대한 항균활성을 측정하였다(도 2 참조).In addition, the general components were analyzed after extraction with each component of the fish and three hundred seconds methanol (see Table 1). In the case of general ingredients, Eoseongcho and three hundred sec showed higher contents than other ingredients, and total vitamin C content was higher than other herbs. In addition, as a result of measuring the free sugar content of eoseongcho and three hundred seconds, the fructose and glucose content was relatively high compared to other green tea leaves and the sugar and maltose content is similar or lower than that of green tea leaves and persimmon leaves (see Table 2). In addition, the antibacterial activity against Bacillus sp . Strains of the fermented extract of Eoseongcho and three hundreds, respectively, were measured (see FIG. 2).
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본 발명에 따른 발효추출물 제조방법은 어성초 및 삼백초의 비린 맛과 향이 제거되면서, 어성초와 삼백초에 함유된 유용성분들을 약리효과의 감소 없이 추출하는 방법을 제공한다.Fermentation extract manufacturing method according to the present invention, while removing the fishy taste and aroma of eoseongcho and three hundred seconds, provides a method for extracting the useful ingredients contained in eoseongcho and three hundred seconds without reducing the pharmacological effect.
이하, 본 발명을 하기 실시예에 의거하여 좀더 상세하게 설명하고자 한다. 단, 하기 실시예는 본 발명을 예시하기 위한 것일 뿐, 본 발명은 하기 실시예 및 첨부된 도면에 의해 한정되는 것이 아니고, 본 발명의 기술적 사상을 벗어나지 않는 범위 내에서 치환 및 균등한 타 실시예로 변경할 수 있음은 본 발명이 속하는 기술분야에서 통상의 지식을 가진 자에게 있어서 명백할 것이다.Hereinafter, the present invention will be described in more detail based on the following examples. However, the following examples are only for illustrating the present invention, and the present invention is not limited by the following examples and the accompanying drawings, and other embodiments equivalent to substitutions and equivalents without departing from the technical spirit of the present invention. It will be apparent to those skilled in the art to which the present invention pertains.
<실시예> <Example>
본 발명자들은 어성초와 삼백초 시료로부터 발효추출물을 제조하였다. 이때, 상기 어성초 및 삼백초는 유기농 재배된 것으로 본 발명자들(세명한방제약(주))이 직접 재배하여 출하한 생체와 건체를 사용하였다. 각종 성분 분석 및 미생물 실험 시약은 경상화공에서 구입하여 사용하였다.The present inventors prepared fermentation extracts from Eochocho and Trichophytium samples. At this time, the Eoseongcho and three hundred vines were organically cultivated, and the present inventors (Semyung Oriental Pharmaceutical Co., Ltd.) used the living bodies and dried bodies grown and shipped directly. Various component analysis and microbial test reagents were purchased from the commercial chemicals.
<실시예 1> 어성초 및 삼백초의 발효숙성액 제조<Example 1> Fermented matured solution of fish and three hundred
본 발명자들은 발효추출물을 다음의 순서로 제조하였다.The present inventors prepared the fermentation extract in the following order.
먼저, 어성초 및 삼백초를 세척한 후 물기를 완전 제거하였다. 이것을 각각 유리항아리에 5㎝정도 넣은 후 설탕시럽을 첨가하고 이것을 계속 반복하였다. 최종적으로 미생물 오염 방지 목적으로 어성초 또는 삼백초가 완전히 덮이도록 설탕시럽을 첨가하였다. 깨끗이 세척ㆍ건조시킨 돌로 눌러서 밀봉시킨 후, 1차 발효를 수행하였다. 생성된 거품을 안정화시키고 2차 발효를 수행하였다. 상온에서 숙성 및 침출(2~3개월)하여 액상물질의 여과액을 발효숙성액으로 사용하였다.First, Echo and three hundred seconds were washed and then completely drained. This was put about 5 cm in each glass jar, sugar syrup was added, and this was repeated. Finally, sugar syrup was added to completely cover edible or triticale for the purpose of preventing microbial contamination. After pressing and sealing with the stone which was washed and dried, primary fermentation was performed. The resulting foam was stabilized and secondary fermentation was performed. After aging and leaching at room temperature (2 to 3 months), the filtrate of the liquid material was used as the fermentation aging solution.
<실시예 2> 발효추출액 제조Example 2 Fermentation Extract Preparation
어성초 및 삼백초에 함유된 유용성분들은 알코올류 등을 통한 추출이 용이하나, 여러해살이풀이 식품 소재로 사용될 경우에는, 유기용매보다 추출수율은 약간 낮으나 안전성과 추출설비 및 제조 단가 등에 장점이 많은 열수를 이용하여 추출하는 것이 바람직하므로 도 1과 같이 추출하였다. 상기 실시예 1에서 제조된 발효숙성액 200g 시료에 증류수 2000㎖을 가한 후 환류냉각기를 부착하여 95℃에서 8시간 열수 추출한 다음 여과하였다. 여액을 50~55℃에서 감압농축기로 전량이 100㎖될 때까지 농축하여 실온까지 냉각한 다음 에탄올을 가하여 75% 에탄올 용액이 되게 한 다음 교반하고 5℃에서 24시간 방치하여 생성된 침전물을 제거한 여과액을 동결건조하여 실험에 사용하였다.The useful ingredients contained in Eoseongcho and Triticalea are easy to extract through alcohols, but when used as a perennial food material, the extraction yield is slightly lower than that of organic solvents, but hot water has many advantages in safety, extraction equipment, and manufacturing cost. It is preferable to extract using, so as shown in FIG. After distilled water 2000ml was added to the fermentation broth 200g sample prepared in Example 1, a reflux condenser was attached and extracted with hot water at 95 ° C. for 8 hours, followed by filtration. Concentrate the filtrate at 50 ~ 55 ℃ to 100ml in a vacuum condenser, cool down to room temperature, add ethanol to 75% ethanol solution, stir and leave at 5 ℃ for 24 hours to remove the precipitate formed. The solution was lyophilized and used for the experiment.
<실시예 3> 어성초, 삼백초의 성분분석<Example 3> Analysis of the components of Eoseongcho, three hundred seconds
상기에서 제조된 어성초 및 삼백초 발효추출물 각각의 일반성분 분석은 AOAC 방법으로 분석하였으며, 시료조제는 시료 1㎏을 분쇄기로 분쇄하고 추출용매인 메탄올과 혼합하여 균질기를 이용하여 균질화 시킨 다음 약 10배량의 메탄올을 3회로 나누어 12시간 동안 반복 추출하였다. 메탄올 추출물은 여과지를 이용하여 여과하고 진공 증발기(vacuum evaporator)를 이용하여 45℃에서 농축하여 사용하였다.Analysis of the general components of each of the Eochocho and Trichocho fermented extract prepared above was analyzed by AOAC method, and the sample preparation was pulverized with 1 kg of sample, mixed with methanol as an extraction solvent, and homogenized using a homogenizer, and then about 10 times The methanol was divided into three times and extracted repeatedly for 12 hours. The methanol extract was filtered using filter paper and concentrated at 45 ° C. using a vacuum evaporator.
그 결과, 어성초 및 삼백초의 화학성분을 분석한 결과는 일반성분 함량은 하기 표 1과 같다. 일반성분의 경우 어성초, 삼백초 공히 다른 성분에 비해 높은 함량을 나타내었으며 총비타민C(아스코빅산) 함량은 다른 약초류에 비해 높은 함량을 나타내었다. 특히, 어성초와 삼백초의 성분차이는 크게 나타나지 않았다.As a result, the results of analyzing the chemical components of Eoseongcho and three hundred seconds, the general component content is shown in Table 1 below. In the case of general ingredients, Eoseongcho and 300baekcho showed higher contents than other ingredients, and total vitamin C (ascorbic acid) content was higher than other herbs. In particular, there was no significant difference between the ingredients of Eoseongcho and 300 sec.
또한, 어성초 및 삼백초의 유리당 함량을 측정한 결과, 표 2와 같이 포도당 0.56%, 과당 0.31%, 설탕 0.05%, 말토스 0.01% 내외로서 다른 녹차잎에 비해서는 과당과 포도당 함량은 비교적 높은 편이었으며 설탕과 말토스 함량은 녹차잎, 감잎에 비해 비슷하거나 그보다 낮은 것으로 나타났다.In addition, as a result of measuring the free sugar content of Eoseongcho and 300 seconds, the glucose content of glucose was 0.56%, fructose 0.31%, sugar 0.05%, maltose 0.01%, and the content of fructose and glucose was relatively higher than other green tea leaves. Sugar and maltose contents were similar or lower than those of green tea and persimmon leaves.
<실시예 4> 어성초, 삼백초 발효추출물의 항균활성 측정Example 4 Determination of Antimicrobial Activity of Fermented Extracts
일반적인 균주 중에서 대표적인 Bacillus속 및 숙성에 관여하는 젖산균에 미치는 영향을 조사하기 위하여 실험균주의 생육배지는 젖산균의 경우 MRS 배지, PDA 배지 등을 이용하여 페이퍼디스크(paper disc) 방법으로 측정하였다.In order to investigate the effect on the representative Bacillus genus and lactic acid bacteria involved in aging among the common strains, the growth medium of the experimental strain was measured by the paper disc method using MRS medium, PDA medium, and the like.
어성초/삼백초 발효추출물을 액상시료로 사용하였으며 생육배지로서 페트리디쉬에 기층용배지(1.5% 한천)를 부어 응고시킨 후 55℃의 수욕상에 미리 플라스크에 준비해 둔 중층용배지(0.75% 한천)에 시험균액(Bacillus subtilis) 일정량(배지:액체배양균=3 ㎖:30 ㎕)을 무균적으로 첨가한 후 혼합하였다. 기층용배지에 중층용배지 3 ㎖를 부어 고르게 도포시켜 응고시킨 것에 추출물을 침지한 디스크를 놓아 밀착시켰고, 0.85% 생리식염수 75 ㎕를 페이퍼디스크에 흡착시켜 생약제추출물이 확산되도록 하였다. 페이퍼디스크를 평판배지 위에 놓아 밀착시켜 4℃ 냉장고에서 1시간 동안 방치한 다음 37℃ 배양기에서 24-48시간 동안 배양한 후 페이퍼디스크 주변의 투명환(clear zone)을 조사하였다. 페이퍼디스크에 의한 항균력 측정한 결과 발효추출물에서는 아무런 세균(Bacillus subtilis) 생육 억제력을 보이지 않았으나 건체추출물에서는 항균활성을 가지는 것으로 보아 발효추출물의 항균성 물질은 발효 중에 소실되는 것으로 생각되며 건체추출물은 일정농도 이상에서는 항균활성을 가진 식품의 기능성을 가진다. 도 2는 어성초 및 삼백초 추출물의 항미생물 활성을 나타낸 사진이다. 도 2의 (a) 및 (c)는 어성초 추출물이고, (b) 및 (d)는 삼백초 추출물이다.The fermented extract of Eoseongcho / Sanchocho was used as a liquid sample, and solidified by pouring a basal medium (1.5% agar) into Petri dishes as a growth medium and then preparing it in a middle-layer medium (0.75% agar) prepared in a flask on a 55 ° C water bath. A certain amount of test bacteria ( Bacillus subtilis ) (medium: liquid culture bacteria = 3 ml: 30 μl) was added aseptically and mixed. 3 mL of medium broth was poured onto the base broth and evenly applied to the solidified medium, and the disc dipped with the extract was brought into close contact. 75 μl of 0.85% physiological saline was adsorbed onto the paper disc to allow the herbal extract to be diffused. The paper disks were placed on a plate medium to be in close contact with each other, and left for 1 hour in a 4 ° C. refrigerator, then incubated for 24 to 48 hours in a 37 ° C. incubator, and then the clear zone around the paper disks was examined. As a result of measuring the antimicrobial activity by paper disc, the fermented extract showed no inhibitory effect on the growth of bacterium ( Bacillus subtilis ), but the dry extract had antimicrobial activity, so the antimicrobial material of the fermented extract was lost during fermentation. Has the functionality of food with antimicrobial activity. Figure 2 is a photograph showing the antimicrobial activity of Echochocho and Trichophytium extract. (A) and (c) of FIG. 2 are extracts from Echochocho, and (b) and (d) are extracts of three hundred sec.
도 1은 Hottuynia cordata 및 Sarurus sinensis로부터 열수 및 에탄올 추출의 제조단계를 요약한 공정도이고, 1 is a process diagram summarizing the preparation steps of hot water and ethanol extraction from Hottuynia cordata and Sarurus sinensis ,
도 2는 Hottuynia cordata 및 Sarurus sinensis의 추출물의 항미생물 활성을 나타낸 사진(이때, (a)는 발효된 Hottuynia cordata(10Brix)이고, (b)는 발효된 Sarurus sinensis(10Brix)이고, (c)는 Hottuynia cordata(10Brix)이고 (d)는 Sarurus sinensis(10Brix)이다)이다. Figure 2 is a photograph showing the antimicrobial activity of the extracts of Hottuynia cordata and Sarurus sinensis (where (a) is fermented Hottuynia cordata (10Brix), (b) is fermented Sarurus sinensis (10Brix), (c) is Hottuynia cordata (10Brix) and (d) is Sarurus sinensis (10Brix).
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JPS57106623A (en) | 1980-12-22 | 1982-07-02 | Hiroshi Sakaguchi | Tea of houttuynia cordata and its preparation |
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JPS57106623A (en) | 1980-12-22 | 1982-07-02 | Hiroshi Sakaguchi | Tea of houttuynia cordata and its preparation |
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