KR100775741B1 - A method for the preparation of extract from Angelica gigantis radix and the composition containing the extract - Google Patents

Abstract

      The present invention relates to a process for preparing a Angelica extract and extracts thereof, in the preparation of the Angelica extract, a carbohydrate such as polysaccharides contained in Angelica is removed, and thus the pharmacological components of Dicursin and Dicusinol. The present invention relates to a method for producing a composition and a composition of the Angelica extract, characterized by increasing the content three times or more.

Angelica, Carbohydrates, Dicusin, Dicusinol

Description

A method for the preparation of extract from Angelica gigantis radix and the composition containing the extract}

Angelica gigantis radix is a perennial herb belonging to the family of the Buttercup (Umbelliferae). In Korea, Japanese donkeys are cultivated and produced in northern Japan, in Gansu, Yunnan, Shaanxi, Sichuan, and Guizhou (Crop Experiment Station, 1998. Test and Research Report (Special and Pharmaceutical Products)). As a medicinal product, it is mainly used for gynecological diseases such as cold and anemia, and it is used to facilitate blood circulation and to improve hematopoiesis and blood flow.

Angelica has been widely used as a medicine to be considered nontoxic in traditional Chinese medicine. In the case of Chinese medicine, extracts extracted from hot water are used. For the study of its effectiveness, Kim Soo-min and others reported antioxidant effects on lipids (Journal of the Korean Society of Food Scoence and Nutrition, 1998.) Radical scavenging activity and antioxidant effects of hot water extracts were reported (2004 Poster presented at the Korean Society for Nutrition and Nutrition, Spring Conference, P4-6; J. Korean Soc.Food Sci.Nutr., 33 (7), 1112-8 , 2004), and Lee Sun-young reported the results of electron donating ability, total phenolic compounds, nitrite removal ability in microwave extract (Food Sci. Biotechnol., 12 (5), 491-6, 2003). Decursin, decursinol, decursionl angelate and essential oils have been reported as ingredients in Angelica extract. For the efficacy of these ingredients, Ahn, Kyung-Seop et al. Reported that the cytotoxicity of the decosinol angelate and deculcin contained in Angelica gigas extract was due to the activation of pretein kinase C (1996 Spring Conference, P89). Et al. Reported anticancer efficacy of these components (Arch. Pharm. Res. 26 (9), 727-30, 2003), and Lee Yong-wook reported the antiplatelet and anticoagulant efficacy of these and nodakenin ( Arch. Pharm. Res., 26 (9), 723-6, 2003), and Kyung-Won Yun et al. Reported the antimicrobial activity using fractions of the organic solvents of methanol extracts of Chaff and Angelica gigas (Korean J. Plant Res. , 17 (3) 278-82, 2004), Lee Sang-Hyun and others reported the antimicrobial activity of methanol extracts (Arch. Pharm. Res. 26 (6), 449-52, 2003). 18.1% (w / w) protein, 8.9% (w / w) lipid, 57% (w / w) carbohydrates (Korean J. Food Sci.Technol., 29 (6), 1113-8, 1997), and Noh Bong-su reported the results of analyzing the fragrance components of Angelica tang using an electronic nose (Surface acoustic wave sensor) (Korean J. Food Sci. Technol., 35 (1), 144-8, 2003), and Cho Min-gu reported the study on the contents of volatile essential oils and their components of Korean Angelica vulgaris (Korean J. Medicinal Crop). Sci., 11 (5), 352-7, 2003), Kwak, Jae-jin and others reported the volatile aroma components of oleoresin in Angelica gigas (J. Korean Soc. Tobacco Sci., 20 (2), 210-7, 1998 ).

In the preparation of Angelica gigas extract, most of them used an organic solvent or water, and in the study related to the identification or observation of efficacy of the extract, fractions using organic solvents were used. Sunyoung Lee studied the microwave process to extract the useful components of Angelica (J. Korean Soc. Food Sci. Nutr., 29 (3), 442-7, 2000). The results of the study on the preparation of ethanol were reported (Korean J. Food & Nutr., 14 (6), 543-7, 2001).

Carbohydrate content is known to be very high, close to 50% by weight of extract (Korean J. Food Sci.Technol., 29 (6), 1113-8, 1997), but monosaccharides such as glucose, fructose and sugar And the content of disaccharides was found to be very small at the level of 0.5% (w / w). This may assume that the sugar component contained is polymeric. Based on this, Young S. Park et al. Reported a study on the differentiation of angelic stem cells, a polysaccharide contained in Angelica gigas (Korean J. Medicinal Crop Sci., 10 (4), 2002).

Angelica has been used as a herbal medicine for a long time, so there are a variety of technologies for which patents have been applied to commercialize related technologies.

Korea Institute of Oriental Medicine suggests an extract for inhibiting the side effects of chemotherapy containing Angelica in Korean Patent 0519456, and Getwell Bio Co., Ltd. in Korea Patent 0427704 for the prevention and treatment of gastric mucosal injury containing decosinol of Angelica Angelica Presenting the composition, Natural Endotech Co., Ltd. is presenting a antagonist composition of dioxins using the Angelica extract in Korean Patent 0480970, Psygene Co., Ltd. painkiller composition containing dicursinol in Korea Patent 0397950 Presented by, Saizen Harvest Co., Ltd. is presenting a hangover relief composition containing dicursinol in Korea Patent 0448680, Lee Sechang prevention and treatment of dementia containing Angelica extract in Korea Patent Application 10-2003-0074646 The present invention provides a composition for the treatment, and Jeong, Se-Young et al. Propose a renal toxicity inhibitor composition containing dicusin in Korean Patent 0504405. Korea Research Institute of Bioscience and Biotechnology proposes a composition for preventing and treating diabetes of Angelan, a polysaccharide isolated from Angelica gigas, in Korea Patent 0441644, and Cygene Co., Ltd. is a decosinol in Korea Patent Application 10-2000-0060196 The present invention proposes a composition for preventing and treating septic shock, which includes a method for preparing useful components of donkey by cultivating a real donkey root cell in Korean Patent 0385092, and Korea Research Institute of Science and Technology Patent 0252194 proposes the isolation of pectin polysaccharides of the Angelica gigas and its use as an adjuvant, and Cheil Pharm. Co., Ltd. in Korea Patent 0187881 proposes a method for producing an anticancer agent containing dicusinol angelate, Korea Food Research Institute Korean Patent 0059142 proposes a method for producing a beverage containing Angelica as a main ingredient, and the Rural Development Administration 0132609 proposes a method for producing a donkey granule tea, and Cho Hyun-jun suggests a method for extracting anti-tuberculosis agent from a donkey in Korean Patent 0003649, and the widow rate suggests a method for producing a donkey extract using petroleum ether and neutral acetate in Korean Patent 0002596 Kim Han-seung proposes an extraction method using a method of adjusting the pH as a method of extracting the essential oil components of Angelica in Korea Patent 0003195, Han Sang-pil, etc., urine containing the Angelica extract in Korea Patent Application 10-2004-0046403 Disorders and edema treatment compositions are proposed, MDI Alpha Co., Ltd. is proposed in the Korean patent application 10-2004-0036199 diabetic therapeutic composition using the Angelica extract, Kim Hyung-wan et al. In Korean patent application 10-2005-0079103 Vasodilators containing dicusin or dicusinol angelate are proposed in ( STC is presenting a composition for preventing or treating dementia or improving cognitive function of an extract containing Angelica in Korean Patent Application No. 10-2005-0087384, Elcom Science Co., Ltd. in Korea Patent Application 10-2004-0008975 It is presenting a composition for improving brain function and cognitive function as a complex extract containing, and the Korea Institute of Science and Technology proposes a decosin as an anticancer agent in Korea Patent 0176413.

The present invention relates to the manufacture of the Angelica extract minimizing the content of carbohydrate components contained in the Angelica Angelica in the preparation of the Angelica extract extract so far, the production of the Angelica extract is not dried and harvested Angelica There is a compression method to obtain an extract by pressing at the method, the device is simple to operate and low yield. Next, there is a method of distillation using water vapor, which is extracted at 100 ° C. or higher, so heat-sensitive components are easily destroyed or decomposed. The extraction method using an organic solvent is very effective for extracting active ingredients, Many, large amounts of energy are consumed in the process of removing the solvent. Extraction method using supercritical fluid is fast extraction speed and can minimize the consumption of solvent, but it is difficult to enlarge the equipment and the equipment is expensive. In addition to the extraction method using a microwave is known, but also has the disadvantages of expensive equipment, relatively difficult to enlarge, and high energy consumption.

Until now, most of the extracts of Angelica gigas were extracted using solvents such as water or ethanol, ether, hexane, etc. The composition of the extracts is mainly simple complex without any refining process, in the form of extracts and mixtures of other medicinal herbs. Most of them were used. Of course, studies on a process for separating polysaccharides separately from the Angelica extract or separating processes such as dicusin, dicusinol, and dicusinol angelate, which are widely known as active ingredients, are also known. However, no research has been reported on the preparation of extracts, including the purification process for preparing the extract of Angelica gigas and increasing the content of dicusin and dicusinol with pharmacological efficacy in the extract state, and the extract has not been reported.

In the present invention, the object of the present invention is to provide a method for producing a Angelica extract minimizing the content of carbohydrate components contained in a large amount in Angelica extract and its extract. Angelica contains a large amount of carbohydrates (polysaccharides, sugars) and when extracted with a solvent such as water, ethanol, these components are extracted at the same time. These components are precipitated by precipitation in the process of concentrating the filtrate obtained after extraction. The present inventors have difficulty in obtaining a homogenized powder as a result of powdering due to precipitation of saccharides which have been precipitated in the process of powdering by adding an excipient to the concentrate obtained in this manner, and in the process of spraying the concentrate on the excipient for powdering. In order to improve the manufacturing process problems such as clogged nozzle due to the precipitation. Due to pharmacological efficacy, the Angelica extract was obtained in a homogenized powder form, which was necessary for the development of various formulations of the product. However, by conventional extraction, the powdering process is difficult due to precipitation of saccharides produced in the concentration process after extraction, and it is not possible to obtain a homogenized powder. Therefore, the process of the present invention has been developed to remove the carbohydrates contained in the extract in advance to solve the problems caused by the powdering process, to obtain a homogenized powder, and to increase the content of dicursin and dicursinol having high pharmacological efficacy. .

Angelica has long been used as a medicinal herb in Chinese medicine, and its efficacy has been researched after analyzing and identifying individual ingredients through the analysis of ingredients by modern science in addition to medical books such as Dongbobom.

The present invention provides a method for obtaining a Angelica extract from which carbohydrates are contained in Angelica in a large amount in preparing Angelica extracts in order to utilize the various pharmacological effects of Angelica as a food, and as a composition obtained therefrom, the content of dicusin and dicusinol. It is an object of the invention to provide a process and composition which is dramatically increased.

Hereinafter, the configuration of the present invention will be described as follows.

The present invention is the extraction process by adding alcohol to the extract as a solvent, extract, concentrate the extract to obtain a primary concentrate, and adding a high-purity ethanol to remove the insoluble carbohydrate in ethanol, and the obtained filtrate is concentrated It consists of the process of removing ethanol and obtaining Angelica extract.

First, in the process of obtaining the primary concentrate, dried Angelica is less than 3% (w / w) of water content, and alcoholic beverage containing 80% (v / v) or more of ethanol equivalent to 2 to 8 times the weight of Angelica. Add and extract for 2-6 hours at a temperature of 40 ~ 70 ℃. In this case, the moisture content of the donkey is dried below 3% (w / w) to minimize the dilution of the added alcohol due to the moisture contained in the donkey during the extraction process by adding alcohol when the moisture content of the donkey increases. The ethanol concentration of 80% (v / v) or higher is intended to increase the extraction of ethanol soluble components and to inhibit the extraction of carbohydrates (saccharides), which are the main components of water-soluble components, to reduce the concentration of ethanol to 80% ( v / v) is not a problem in making an extract, but there is a difference that excess carbohydrates are extracted, and in the case of alcohol where the concentration of ethanol is normally obtained, the highest concentration is 95% (v / v). Did not set. When the amount of alcohol added is 2 to 8 times the weight of donkey, donkey is generally bulky compared to the weight because it is sold in small pieces. However, when the amount of solvent is small, the donkey cannot be sufficiently submerged. This leads to the use of excessive solvents. The extraction temperature was set at 40 ° C. or higher in consideration of extraction efficiency, and the boiling point of ethanol was 78 ° C., and thus 70 ° C. or lower was determined as the upper limit. Of course, higher temperatures are possible, but in that case, the boiling point of ethanol will be higher, and the risk is very high due to excessive vapor pressure. In addition, higher temperatures than necessary will result in the destruction of the weak components of the heat. When the extraction time is less than 2 hours, yield decrease occurs, and in the case of more than 6 hours, there is no further improvement in yield, and it is determined to be between 2 hours and 6 hours. After the extraction was completed, the filter was filtered using a 10 micron pore to completely remove fine insoluble components, and the filtrate was concentrated in vacuo to obtain a fully concentrated concentrate. To this, ethanol having a purity of 95.5 to 99.9% (v / v) was added 3 to 6 times the weight of the obtained concentrate, and redissolved at 40 ° C. In this process, soluble components are dissolved, but carbohydrates insoluble in ethanol remain in the form of precipitation. After sufficient dissolution, it is left at a temperature of 5 to 10 ° C. for at least 2 hours. In this process, some redissolved sugars are reprecipitated by sedimentation. This was again filtered through a 10 micron filter to remove precipitated carbohydrates, and the filtrate was obtained to complete the carbohydrate removal process. The filtrate is concentrated in vacuo to complete the process of completely removing the solvent to obtain a sugar extract extract containing a minimum of carbohydrate components. Here, the minimum means that the trace amount of carbohydrate (0.1-4.5% in the solvent, v / v) contained in the solvent used can be dissolved in the trace amount of carbohydrates, so that the carbohydrates are not included at all.

The solvent used in the carbohydrate removal process is to make ethanol purity 95.5 ~ 99.9% (v / v) to minimize the solubility of carbohydrates. Because it becomes. Best of all, using 99.9% ethanol is the way to minimize sugar content. The volume of ethanol added should be at least 3 times and not more than 6 times in sufficient quantity to extract soluble components. Doing more than 6 times increases the dissolution of sugars due to the water in ethanol. After dissolution, it is left for 5 hours at 5 ~ 10 ℃ to precipitate the dissolved sugar in the process of dissolving at 40 ℃, to grow the obtained sugar crystals to facilitate filtration. This is because the temperature to be left is 5 to 10 ° C. and lower than that, but the viscosity of the solution increases due to the low temperature, and as a result, the filtration is not easy. Of course, when using a method such as centrifugation instead of filtration, stationary conditions of 5 ° C or less are not a problem. The time to leave is 2 hours, which is enough time for the contents to cool down, which is enough time for the precipitation of saccharides to be formed, and even more than 2 hours for 20 hours has no effect on the process. A 10 micron filter was used as a method of removing the precipitate formed after standing, but a method such as centrifugation may be used. The pore size of the filter used was set to 10 microns because most of the saccharide precipitates could be removed based on the clarity of the liquid obtained from the filtration. As a result, the removed carbohydrate was able to remove most sugars from 85% to 99% based on the analysis of sugars in food industry. The elimination of sugar here does not necessarily have to be perfect. However, if the sugar can eliminate the possibility of process problems and increase the content of the active ingredient in the extract to the level required by the product may be regarded as a problem solved.

The obtained Angelica extract was more than three times higher than the extract obtained by the conventional simple extraction method of dicusin and dicusinol, which are known as effective pharmacological components, more than 30% (w / w). Was 0.25% (w / w), more than three times higher than the simple extraction method. In order to facilitate powdering, more than 35% (w / w) of MCC (micro crystalline cellulose) as an excipient was prepared and dried by spraying to obtain a homogenized yellow Angelica extract powder. There was no clogging of the spray nozzles that occurred when using the conventional extract. In addition, when preparing the Angelica extract powder using the extract of the present invention, compared to the case of using an extract containing a large amount of conventional carbohydrates, the content of dicusin, dicusinol, dicusin angelate known as an active ingredient per powder is minimal Since it can be increased more than two times, the amount of donkey extract powder to be eaten in order to ingest the donkey extract containing the same active ingredient could be reduced to less than 1/2. This means that if the existing Angelica extract should be ingested four capsules per day, the extract of the present invention is sufficient to intake only two capsules. This can be very important for older or patients. In addition, it may be a decisive factor if the intake needs to be doubled or tripled as needed. In other words, the existing extract should be taken 4 times a day, meaning that 2 times of ingestion is enough, so when the product is released to the market, it can be a decisive factor for the buyer to choose. This can be said.

Hereinafter, the following examples will be described as an example of the present invention. However, this embodiment does not limit the scope of the present invention.

Example 1.

2Kg of Angelica Angelica was purchased from Gyeongdong Market and further dried in an oven at 60 ℃ for 6 hours to make water content 2.5% (w / w), of which 500g was taken to make alcohol with 85.1% (v / v) ethanol concentration. 6 times 3,000 ml were added and extracted for 4 hours at a temperature of 60 ° C. After the extraction was filtered to give 2610 ml of the extract. The solvent was removed by concentration under vacuum of 15 mmHg absolute pressure. As a result, 180 g of primary concentrate was obtained. 96% (v / v) of ethanol was added to 540 ml corresponding to three times the primary concentrate and redissolved at 40 ° C. Most of the dark brown material in the primary concentrate was redissolved and a white precipitate formed. It was left at 8 ° C. for 2 hours to form a precipitate of additional sugars. The precipitate was filtered through a filter paper to remove precipitate, and the filtrate was concentrated in vacuo to obtain 67 g of dark brown transparent Angelica extract. The sugar removed in this process was 113 g.

Example 2.

400 g of the re-dried Angelica gigas obtained in Example 1 was taken and 5 ml of ethanol having a ethanol concentration of 90.1% (v / v) was added thereto and extracted at a temperature of 63 ° C. for 5 hours. After the extraction was filtered to give 1590 ml of the extract. This was concentrated under vacuum at 10 mmHg of absolute pressure to remove the solvent. As a result, 85 g of primary concentrate was obtained. To this was added 255 ml of 99% (v / v) ethanol corresponding to three times the primary concentrate, and redissolved at 40 ° C. Most of the dark brown material in the primary concentrate was redissolved and a white precipitate formed. It was left at 10 ° C. for 2 hours to form a precipitate of additional sugars. Then, the resultant was filtered through a filter paper to remove the precipitate, and the filtrate was concentrated in vacuo to obtain 48 g of dark brown transparent Angelica extract. The sugar removed in this process was 37g.

Example 3.

Dissolve by adding 100 ml of 95% (v / v) alcohol to 50 g of the extract of Example 1, 40 g of MCC (micro crystalline cellulose) was added to a pre-prepared circulating dryer, and the extract through a line equipped with a fine spray nozzle. It was mixed and dried while feeding. As a result, 94g of yellow Angelica extract powder was obtained, and no process problems occurred.

Example 4.

1g of the Angelica extract obtained in Example 2 was hydrolyzed for analysis of sugars by the method of the food industry, and the sugar content was analyzed by HPLC, and the total sugar content was 1.2% (w / w), which was the above example. 1.8% of the sugar content of the first extract of 64.3% (w / w) can be seen that 98.2% of the sugar was removed.

Example 5.

In order to compare the pharmacological component content of the extract of Example 2, 30 g of the dried donkey of Example 1 was added 10 times multiples of 80% (v / v) and extracted at 70 ° C. for 4 hours, and the extract obtained by concentrating the filtrate, The main pharmacological components in 12 g were compared. As a result of the analysis of dikersinol and dikersin reported as major medicinal ingredients in Angelica gigas extract by HPLC (analysis method: Ryu, KS, Korean J. Pharmacogn., 21, 64-8 (1990)) As shown, the extract of the present invention was 3.76 times higher dickerin, 4.27 times higher dicusinol was found to contain a high content of active ingredient by weight.

table. Analysis result of the content of the active ingredient in the extract (%, w / w)

sample Dickin Dicursinol Extract of the invention 42.1 0.38 80% spirit extract 11.2 0.089

The present invention relates to a method for obtaining a obtained Angelica extract obtained by removing carbohydrate components (polysaccharides, sugars) contained in a large amount in Angelica in the preparation of Angelica extract, and according to the process of the present invention, Due to excessive carbohydrates (saccharides) precipitated in the process of powdering, it completely eliminates nozzle clogging in operation and disproportionation of the product, and extracts Angelica extract containing high concentrations of active ingredients such as decurcin and dicursinol. It provides a way to make it into powder form. It is very easy to commercialize, since it can reduce the external volume of extracts taken once or daily per day when preparing Angelica extract as health functional food, food ingredients, etc. It is also easy to commercialize various pharmacological agents such as anticancer drugs, dementia treatment agents, and immunostimulants. It can contribute to the promotion of national health by making the most of the benefits.

Claims (4)

A process for preparing a Angelica extract, comprising a process for obtaining a primary concentrate, a carbohydrate removal process, and a process for obtaining a Angelica extract, 1) In the process of obtaining the primary concentrate, dry the Angelicae and make the water content less than 3% (w / w), and add alcohol of 80% (v / v) or more with ethanol purity 2 to 8 times the weight of the Angelicae. , Extracted for 2-6 hours at a temperature of 40 ~ 70 ℃ to obtain a filtrate, and concentrated in vacuo to remove the solvent, and to obtain a concentrate, 2) In the process of removing carbohydrate, add 3-6 times the weight of the concentrate obtained from 95.5 to 99.9% (v / v) ethanol to the concentrate obtained in the process of obtaining the primary concentrate, and redissolve at 40 ° C. Then, it is left for 2 hours or more at a temperature of 5 ~ 10 ℃ to form a carbohydrate crystals and then filtered through a filter of 10 microns to remove the precipitate of precipitated carbohydrates, and to obtain a filtrate, 3) The step of obtaining the Angelica extract is obtained by the method of vacuum concentrating the filtrate from which the obtained carbohydrate has been removed to completely remove the solvent, Method for producing a Angelica extract, characterized in that. The extract obtained in claim 1, wherein the content of dickerin is 30% (w / w) or more, and the content of dicursinol is 0.25% (w / w) or more. A composition for food containing the extract obtained in claim 1 as a main component. The Angelica extract, characterized in that the amount of carbohydrate removed in 2) of claim 1 is at least 85% (w / w) of the total amount of carbohydrate in the concentrate.