JP2000351801A - Highly pure fucoidan and preparation thereof - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide a highly pure fucoidan which is obtained using a seaweed such as Cladosiphon okamuranus, etc., as a raw material and has a reduced color development or seaweed odor, and a preparation process thereof. SOLUTION: A highly pure fucoidan is prepared through a process comprising steps wherein a) a hot water extract or acid extract of a seaweed is either frozen and then re-melted or dried and then redissolved, and b) an alcohol is added to the re-melted or redissolved, hot-water or acid extract of a seaweed to remove a precipitation. A food product, a pharmaceutical or a cosmetic contains this.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

The present invention relates to a high-purity fucoidan, and more particularly, to a high-purity fucoidan from which colored substances derived from raw algal cells and a unique flavor (seaweed odor and taste) are removed or reduced, and a production thereof. The present invention also relates to a method and a medicament and a cosmetic such as a prophylactic / therapeutic agent for gastrointestinal ulcer containing the high purity fucoidan.

[0002]

2. Description of the Related Art Fucoidan, a sulfated polysaccharide containing fucose as a main constituent sugar, has an antiulcer effect and an effect of inhibiting adhesion of Helicobacter pylori, which is a causative bacterium of gastric ulcer, etc., to the stomach wall. It is expected that it can be added and taken daily to help prevent and treat gastric diseases (Japanese Patent Application Laid-Open No. 7-138166). This fucoidan is particularly useful for the warm sea marine brown algae Okinawa mozuku (C
ladosiphonokamuranus TOKI
DA) It is contained in a large amount as a component of algal bodies such as algae. Fucoidan contained in this Okinawa mozuku is α1
-3 is a polysaccharide having a structure in which a uronic acid residue is bonded to a part of a sugar chain composed of fucose and sulfated fucose, and also partially contains an acetyl group.

[0003] Fucoidan can be easily obtained from an algal body by means of hot water extraction, acid extraction or the like, and can be easily obtained. The hot water or acid extract of algae such as okinawa mozuku produced using this easy extractability is a material which has a high fucoidan content and can be sufficiently used in the above-mentioned applications as it is in terms of the content.

However, many of these extracts are strongly colored with pigments derived from algae. For example, the extract of Okinawa mozuku is colored brown, so that when it is to be incorporated into foods and the like, There is a disadvantage that the appearance and properties of the product are adversely affected.

[0005] Further, since these extracts have a strong flavor (seaweed odor and taste) peculiar to seaweed, they also have a disadvantage that they adversely affect the flavor and properties of foods and the like to which they are added.

[0006] It is very difficult to solve the above-mentioned problems that hinder the use of fucoidan as a food material. For example, activated carbon widely used in the food field for reforming decolorization, deodorization, correction of unpleasant taste, and the like. , Porous adsorption resin, ion exchange resin,
It has been considered that treatments such as electrodialysis and ultrafiltration have little effect on decolorization or deodorization of the extract.
Recently, the present applicant has proposed a method for improving the quality of a mozuku extract containing fucoidan by subjecting mozuku or an extract thereof to a hydrogen peroxide treatment (Japanese Patent Application Laid-Open No. Hei 10 (1998)).
191940). Although this method itself is excellent, from the viewpoint of promoting the use of seaweed such as mozuku as a fucoidan source, it has been required to provide another method.

[0007]

SUMMARY OF THE INVENTION Accordingly, an object of the present invention is to provide a high-purity fucoidan obtained by using seaweed such as Okinawa mozuku as a raw material and having reduced coloring and seaweed odor, and a method for producing the same. .

[0008]

Means for Solving the Problems The present inventors have conducted intensive studies in order to solve the above-mentioned problems. As a result, the extract from seaweed is once frozen or dried, and then alcohol is added to remove impurities. The present inventors have found that high-purity fucoidan that has been removed and substantially decolorized and deodorized can be obtained, and the present invention has been completed.

That is, the present invention provides the following steps a) and b), a) a step of rethawing a hot water extract or an acid extract of seaweed by freezing or drying and re-thawing; b) An object of the present invention is to provide high-purity fucoidan produced by a method comprising a step of adding an alcohol to the re-melted or re-dissolved hot water or acid extract of seaweed to remove a precipitate.

The present invention also relates to the following steps a) and b): a) a step of rethawing a hot water extract or an acid extract of seaweed by freezing or re-thawing by drying; b) It is intended to provide a method for producing high-purity fucoidan, which comprises a step of adding an alcohol to the re-melted or re-dissolved hot water or acid extract of seaweed to remove a precipitate.

Further, the present invention also provides a medicament containing the above-mentioned high-purity fucoidan as an active ingredient, such as a preventive / therapeutic agent for gastrointestinal ulcer, and a cosmetic containing the high-purity fucoidan.

[0012]

BEST MODE FOR CARRYING OUT THE INVENTION The seaweed used as a raw material for producing the high-purity fucoidan of the present invention is not particularly limited as long as it contains fucoidan. Alamiaceae, sea turtle family, sea urchin family, scorpion family, kelp family, sargassin family, scutellaria family, sibertaceae family, scorpion family,
Brown algae such as Macabaceae, Wakameidae, Honeyscomb family, Lysirubidae, Ainuwakameidae, and Hondaraceae are exemplified.

Among the above-mentioned seaweeds, Okinawa spruce, which is a member of the family Pineaceae, is preferable because it has a high fucoidan content and high decolorization and deodorization efficiency.

The fucoidan extract as a raw material for obtaining the high-purity fucoidan of the present invention is obtained by subjecting fucoidan to hot water extraction or acid extraction by a conventional method. Here, the hot water extraction can be carried out under any conditions by a known method such as the method described in the above-mentioned JP-A-7-138166. Preferably, hot water of about 90 to 100 ° C. is added to the seaweed weight by 0.5. The extraction may be performed for about 60 to 120 minutes (hour) using up to 3 times the amount.

In the acid extraction, seaweed is reduced to about 1% of its wet weight.
Disperse in ~ 3 times the amount of water and add acid to adjust the pH to 2-4, preferably 2-3, then heat to about 50 ° C or more, preferably about 80-100 ° C to elute fucoidan It is implemented by doing. Examples of acids that can be used for acid extraction include hydrochloric acid, acetic acid, and sulfuric acid.

The obtained seaweed extract with hot water or acid (hereinafter sometimes simply referred to as “extract”) is subjected to a treatment such as centrifugation or filtration, if necessary, to remove an insoluble extraction residue. It is preferable to remove it, and if necessary, further purification means such as ultrafiltration or water washing can be performed.

The extract prepared by these methods may have a concentration of 2 to 3% by weight, depending on the type of seaweed and the degree of purification.
It can be obtained in liquid or powder form containing about 0% by weight of fucoidan, and any of them can be used as a raw material for obtaining the high-purity fucoidan of the present invention.

In order to obtain the high-purity fucoidan of the present invention, in step a), the above extract is frozen and then re-thawed, or dried and redissolved.

The conditions for the freezing and rethawing treatment are not particularly limited, and it is sufficient that the extract is cooled and frozen by a conventional method, and then left at room temperature or heated to be thawed. .

The drying and re-dissolving treatment can be carried out by a conventional method. The extract is dried by a known drying means such as freeze-drying or spray-drying, and then dried with an optional solvent such as water.
What is necessary is just to dissolve in hot water etc.

Next, as the step b), the freezing in the step a)
The re-melted or dried / re-dissolved extract is treated with alcohol. By this step, the coloring substance in the extract is precipitated, and this can be fractionated and removed.

The type of alcohol added to the extract in step b) is not particularly limited, but monohydric alcohols having 3 or less carbon atoms, such as ethanol, are particularly excellent in terms of the decolorizing effect. It is preferable because it has an excellent precipitation forming effect. In addition, when the extract after decolorization is used as a concentrate such as syrup without drying, it is necessary to further concentrate under reduced pressure for alcohol removal and concentration in the subsequent manufacturing process, and at this time, the alcohol concentration increases with the concentration. However, from the viewpoint of food hygiene, ethanol is particularly preferable, since a small amount always remains dissolved in water as an azeotrope.

The conditions for the alcohol treatment vary depending on the type of seaweed used as a raw material, but it is preferable to carry out the treatment in such a manner that the carbohydrate concentration in the extract is generally in the range of about 1 to 50% by weight. The upper limit of the carbohydrate concentration may be a concentration range that can maintain fluidity. For example, when Okinawa mozuku is used as a raw material, the carbohydrate (mostly fucoidan) in the extract solution is a polymer substance, If the carbohydrate concentration is high, the mixing with the alcohol tends to be uneven due to the high viscosity, and it takes a long time to recover the liquid volume due to the viscosity. On the other hand, when the carbohydrate concentration is lowered, the amount of alcohol used increases with an increase in the amount of liquid, which is not the best in terms of economy. For this reason, the carbohydrate concentration of the extract is preferably in the range of about 1 to 30% by weight, particularly about 3 to 20% by weight, and more preferably in the range of about 5 to 10% by weight.

The amount of alcohol added depends on the carbohydrate concentration in the extract, but the alcohol concentration after addition is about 20 to 60% (V / V), especially 25 to 50% (V / V).
/ V), and more preferably in the range of about 30 to 45% (V / V). If the alcohol concentration in the extract (final alcohol concentration) is within the above range, only the coloring substance can be easily precipitated, and the decolorizing and deodorizing effects are high.
Fucoidan, the main component, does not precipitate and precipitate,
Fucoidan is fully recovered in the alcohol-water phase. When the carbohydrate concentration of the extract is high, 50% (V
/ V) or more, the fucoidan begins to precipitate when the alcohol is added, and at an alcohol concentration of about 75% (V / V), fucoidan is completely precipitated and recovered. Alcohol treatment can also be used as a purification method.

Further, the pH of the solution at the time of alcohol fractionation
Is preferably in the range of pH 3 to 7, and it is desirable to avoid treatment under strong acidity and on the alkaline side in order to prevent decomposition or recoloration of fucoidan. Furthermore, the temperature at the time of alcohol fractionation is preferably around room temperature (10 to 30 ° C.), and there is no need to cool or heat. It is sufficient for the precipitate formation time to stand for about 30 minutes after the addition of the alcohol and stirring.
If the final alcohol concentration is within the above range, the intended fucoidan itself does not precipitate.

The precipitate produced by the alcohol treatment is:
According to a conventional method, it can be fractionated and removed from fucoidan by means such as filtration and centrifugation.

In the present invention, alcohol treatment can be carried out in the presence of a salt as step c) instead of step b).
Step c) is carried out in the same manner as in step b) above, except that a salt coexists in the alcohol treatment. The type of salt added to the extract in step c) is not particularly limited, and examples thereof include water-soluble monovalent and divalent metal salts such as common salt, calcium chloride, and magnesium chloride. When blending high-purity fucoidan in foods, etc., it is preferable to use edible salts as salts, because there is no particular safety problem, there is no need to remove it from the final product, and high-purity products are inexpensive and easy to use. It is approved as a food additive for reasons such as availability,
It is preferable to use calcium chloride or the like.

The amount of salt added to the extract and allowed to coexist is as follows:
About 0.2 to 300% by weight of carbohydrates in the extract,
In particular, the content is preferably about 50 to 100% by weight. At this time, the salt concentration in the extract itself to be treated is taken into consideration, and the salt concentration can be adjusted to the above-mentioned range by adding or reducing salt as needed.

The above-mentioned salts (especially salt) and alcohols (especially ethanol) can be left in foods and cosmetics if they are in small amounts.
By performing the combination of electrodialysis and ultrafiltration, or electrodialysis and reduced-pressure concentration, removal or reduction to an arbitrary degree can be performed.

The high-purity fucoidan of the present invention obtained as described above is obtained by removing or reducing a coloring substance and / or a seaweed odor component derived from seaweed. It can be done by measurement. That is, when the seaweed extract is decolorized, the purity is determined by measuring the absorbance at 520 nm of the extract before and after the treatment and calculating the decolorization rate according to the following equation.

[0031]

## EQU1 ## Decolorization rate (%) = (AB) × 100 / A A: Absorbance of initial liquid (absorbance before decolorization) B: Absorbance of decolorization liquid (absorbance after decolorization)

If the decolorization rate is about 70% or more, it can be determined that the color has been decolorized and the seaweed odor has been removed or reduced to a level that does not hinder the use of fucoidan for various uses. When used as cosmetics, it is desirable to decolorize to about 90% or more. Needless to say, depending on the use of fucoidan obtained by the method of the present invention, it may not be necessary to purify to such high purity.

The high-purity fucoidan obtained by the method of the present invention can be used alone or in combination with other commonly used components for various uses such as foods, pharmaceuticals, quasi-drugs, and cosmetics. It is possible to use.

For example, when the high-purity fucoidan of the present invention is used for foods, sugars such as sugar and fructose, stabilizers, acidulants (citric acid, malic acid), vitamins, minerals and the like are blended. It can be used in the form of tea, coffee, juice drink, fermented milk, carbonated drink, pudding, jelly and the like. In addition, for example, in the case of a drug such as an anti-ulcer drug, the dosage form and dosage can be appropriately selected according to the purpose, but preferably together with a pharmaceutically acceptable liquid or solid carrier, Depending on the solvent, dispersant, emulsifier, buffer, stabilizer, excipient, binder, disintegrant, lubricant, etc. are blended and formulated into tablets, granules, powders, powders, capsules, etc. Can be used. Further, when used as cosmetics, known cosmetic components such as water, alcohols, oil components, surfactants, water-soluble polymers, vitamins, preservatives, fragrances, pigments, and the like are appropriately compounded, It can be used in the form of water, emulsion, moisturizing cream, cleansing cream, massage cream, face wash cream, pack, serum, and the like.

[0035]

The physicochemical structure of a coloring substance to be removed in the present invention (that is, a component which is extracted from algal cells together with fucoidan by hot water or an acid and migrates into the extract) is not clear, but sephacryl ( Sephary
1) It has been found that the polymer has a size that elutes in a portion that passes through gel filtration using S-300 (manufactured by Amersham Pharmacia Biotech). As described above, this coloring substance could hardly be removed by known purification means.

On the other hand, the method of the present invention comprises treating a seaweed extract having been subjected to a specific pretreatment with an alcohol in the presence of an appropriate concentration of a salt to thereby minimize the loss of fucoidan while minimizing the loss of fucoidan. Is preferentially precipitated and separated, thereby enabling the production of high-purity fucoidan which has not been obtained before. Further, as the coloring substance is reduced or removed, the unique seaweed flavor can be significantly reduced.

[0037]

Next, the present invention will be described in more detail with reference to examples and test examples, but the present invention is not limited by these examples. EXPERIMENTAL EXAMPLE 1 Decolorization rate of unfrozen and dried salted mozuku extract (carbohydrate concentration: 1.32% by weight): salted okinawa mozuku (19
(Katsuren 1997) Sprinkle water on 75 kg for washing, then add 100 liters of tap water, add hydrochloric acid (2M) to adjust the pH to 3.0, then heat to 95-98 ° C for 60 minutes and fucoidan component Was extracted. After cooling, the mixture was neutralized to pH 6.0 with sodium hydroxide (1M) and centrifuged to obtain 170 liters of an extract. Using this extract, a decolorization test using salt and ethanol was performed according to the following procedure.

A total of 24 samples each of 50 ml of an extract having a carbohydrate concentration of 1.32% by weight (salt concentration of 2.6% by weight) were taken, and salt was added in an amount of 1%, 5% and 10% by weight for 6 samples. Then, the salt concentration was 2.6% by weight (no addition),
It was adjusted to 3.6%, 7.6% and 12.6% by weight. In addition, 25% for each salt concentration sample,
Ethanol was added to give 30%, 35%, 40% and 45% (V / V) concentrations. In addition, one sample without ethanol was prepared for each salt concentration.

After each sample was sufficiently stirred, it was allowed to stand at 25 ° C. for 60 minutes to form a precipitate. Then, after removing the precipitate by centrifugation, the supernatant volume was adjusted to 100 ml,
The absorbance at 520 nm was measured, and the decolorization rate was calculated based on the above formula. The results are as shown in Table 1. The coloring substances in the extract of salted mozuku did not undergo step a) and hardly precipitated, and only 12.6 of the salt and ethanol of step b) were added. About 5% for an ethanol concentration of 45% (V / V) in the presence of
Only a 0% bleaching rate was obtained.

[0040]

[Table 1]

EXPERIMENTAL EXAMPLE 2 Decolorization rate of unfrozen and dried unprocessed mozuku extract (carbohydrate concentration 1.31% by weight): raw okinawa mozuku (19
(98, Chinen) 100 kg of tap water was added to 75 kg, the pH was adjusted to 3 with hydrochloric acid, and heat extraction was performed at 95 to 98 ° C. for 60 minutes. After cooling, the mixture was neutralized and subjected to centrifugal filtration to obtain an extract. It was then concentrated under reduced pressure to a carbohydrate concentration of 1.3.
86 liters of an extract having a concentration of 1% by weight and a salt concentration of 1.3% by weight was obtained.

A total of 24 samples of this extract were taken in 50 ml portions, and salt was added in an amount of 1%, 5% and 10% by weight in 6 samples, and the salt concentration was 1.3% by weight (no addition). 2.3%, 6.3% and 11.3% by weight
Was adjusted. In addition, two samples were added to each salt concentration sample.
5%, 30%, 35%, 40% and 45% (V / V)
Ethanol was added to a concentration. In addition, one sample without ethanol was prepared for each salt concentration.

After thoroughly stirring each sample, the sample was allowed to stand at 25 ° C. for 60 minutes to form a colored substance precipitate. Then, after removing the precipitate by centrifugation, each test solution was
The volume was adjusted to 0 ml, and the absorbance at 520 nm was measured in the same manner as in Experimental Example 1 to calculate the decolorization rate. The results are as shown in Table 2. When the step a) was not carried out and only the step b) was carried out, the decolorization test of the raw mozuku extract did not exceed 10% in the same manner as in the case of the salted mozuku extract of Experimental Example 1. 45% in the presence of
At an ethanol concentration of (V / V), only a decolorization rate of about 50% was obtained.

[0044]

[Table 2]

EXPERIMENTAL EXAMPLE 3 Decolorization rate of a sample solution (carbohydrate concentration: 6.30% by weight) which had not been subjected to freezing and drying: from salted okinawa mozuku,
The extract prepared according to the method of Experimental Example 1 was adjusted to pH 3 (2M hydrochloric acid), and then subjected to an ultrafiltration module having a molecular weight cut off of 6,000 (manufactured by Asahi Kasei Corporation, SIP-1013, 2,000).
cm ² ). Next, deionized water was added to the concentrate, and the mixture was adjusted to pH 3 and filtered under pressure. Then, purified water was further added and filtered under pressure to prepare a purified concentrate (carbohydrate concentration: 6.30% by weight). .

A total of 24 samples each of 50 ml each of this concentrate were taken, and 6% of salt was added at 1%, 5% and 10% by weight in the same manner as in Experimental Example 1 to reduce the salt concentration to 0% by weight. 1% by weight, 5% by weight and 10% by weight
Was adjusted. In addition, two samples were added to each salt concentration sample.
5%, 30%, 35%, 40% and 45% (V / V)
Ethanol was added to a concentration. In addition, one sample without ethanol was prepared for each salt concentration.

After sufficiently stirring each sample, the sample was allowed to stand at 25 ° C. for 60 minutes to form a precipitate. Next, after removing the precipitate by centrifugation, the volume of each test solution was made constant to 100 ml, and the absorbance at 520 nm was measured as in Experimental Example 1 to calculate the decolorization rate. The results are as shown in Table 3,
No decolorization in the absence of salt or low ethanol concentration,
Only when the final ethanol concentration exceeded 45% (V / V) in the presence of 5% by weight and 10% by weight of salt, decolorization rates of about 50% and 77%, respectively, were obtained.

[0048]

[Table 3]

EXPERIMENTAL EXAMPLE 4 Decolorization rate of frozen and thawed raw okinawa mozuku extract (carbohydrate concentration 2.70% by weight):
The extract prepared according to the method of Experimental Example 1 was treated in the same manner as in Experimental Example 3. That is, the extract was subjected to ultrafiltration, deionized water was added to the obtained concentrate, adjusted to pH 3, filtered under pressure, purified water was added, and filtered under pressure to obtain a purified concentrated solution.

The obtained concentrated concentrate was stored in a low-temperature warehouse (−30).
° C) and frozen, then immersed in running water to thaw.
The melt was diluted to a solids concentration (carbohydrate concentration) of 2.70% by weight, and 24 samples of 50 ml each were collected. As in Experimental Example 1, salt was added in an amount of 1%, 5% and 10% by weight in the same manner as in Experimental Example 1, and the salt concentration was reduced to 0% by weight (no addition), 1% by weight, 5% by weight and 10% by weight.
Was adjusted. In addition, 25%, 30
%, 35%, 40% and 45% (V / V) ethanol was added. In addition, one sample without ethanol was prepared for each salt concentration.

After thoroughly stirring each sample, the sample was allowed to stand at 25 ° C. for 60 minutes to form a precipitate. Next, after removing the precipitate by centrifugation, the volume of each test solution was made constant to 100 ml, and the absorbance at 520 nm was measured as in Experimental Example 1 to calculate the decolorization rate. The results are as shown in Table 4,
Addition of ethanol in the absence of salt did not cause any decolorization, but addition of ethanol in the presence of salt resulted in a decolorization rate of 90% or more. Fucoidan having a 90% bleaching rate is a material having a coloring degree that does not hinder practical use.

[0052]

[Table 4]

EXPERIMENTAL EXAMPLE 5 Decolorization rate of frozen and re-thawed salted mozuku extract: Experimental example 3
According to the method described above, a concentrate was prepared through extraction and purification steps using salted mozuku as a starting material. This concentrate was frozen in a low-temperature warehouse (-30 ° C.), immersed in running water and thawed to adjust the carbohydrate concentration to 1.25% by weight and 2.90% by weight. Decolorization was performed according to the method. The results are shown in Table 5 when the carbohydrate concentration is 1.25% by weight, and in Table 6 when the carbohydrate concentration is 2.90% by weight.

[0054]

[Table 5]

[0055]

[Table 6]

EXPERIMENTAL EXAMPLE 6 Decolorization rate of dried and redissolved salted mozuku extract: According to the method of Experimental Example 3, a concentrated product was prepared through extraction and purification steps using salted mozuku as a starting material. After the concentrate was spray-dried, it was dissolved in deionized water to adjust the carbohydrate concentration to 5.0% by weight and 10.0% by weight, and the color was decolorized according to the method of Experimental Example 2 for each. The results are shown in Table 7 for those having a carbohydrate concentration of 5.0% by weight, and for those having a carbohydrate concentration of 5.0% by weight.
Are shown in Table 8, respectively.

[0057]

[Table 7]

[0058]

[Table 8]

EXPERIMENTAL EXAMPLE 7 Recovery rate of fucoidan of decolorized liquid of salted mozuku extract dried and redissolved after drying: using the 10% by weight carbohydrate concentration solution of Experimental example 6, and changing the alcohol concentration to a higher concentration. Was performed and the recovery rates of fucoidan were compared. Table 9 shows the results.

[0060]

[Table 9]

Test Example 1 (1) Change in physical quantity before and after decoloration: salted okinawa mozuku (1
200 kg of tap water was added to 176 kg of Katsuren, Okinawa Prefecture, 997; salted mozuku, and the pH was adjusted to 3.0 with hydrochloric acid (2M), followed by extraction at 95 to 98 ° C for 90 minutes. After cooling, the pH was adjusted to 5.5 with sodium hydroxide (1M), and filtered with a filter press to obtain an extract. Next, the extract was slightly desalted by electrodialysis and then spray-dried to produce 2,280 g of a powder having a water content of 7%, a carbohydrate content of about 79%, and a salt content of about 14% by weight (hereinafter, referred to as the following). ,
Described as "crude extract").

730 g of the above crudely purified extract (derived from about 60 kg of salted mozuku) was redissolved in tap water to give a total amount of 5,800 m
1 (10% w / w carbohydrate concentration) and 45%
(V / v) Ethanol was added to give a concentration, and the mixture was allowed to stand at room temperature (25 ° C.) for 60 minutes. The resulting precipitate was removed by centrifugation to obtain a supernatant.

The obtained supernatant was washed with tap water for 12,000 m.
and then adjust 2,000 ml to pH 3.0 (2
M hydrochloric acid), and further diluted to 5,000 ml and subjected to ultrafiltration (fraction molecular weight: 6,000, SIP-1013, 2,000).
cm ² , manufactured by Asahi Kasei Corporation). In this concentrate,
After adding 5,000 ml of deionized water, the mixture was adjusted to pH 3.0 and concentrated under pressure.

Next, 5,000 m of purified water was added to the concentrate.
1 and concentrated under pressure. This operation of adding water and concentrating was repeated until no salt was observed in the filtrate, and finally the concentrate was freeze-dried. The purification operation by ultrafiltration was repeated in the same manner for the remaining 10,000 ml of ethanol supernatant,
High-purity fucoidan powder (product of the present invention) in total 282.2 g
Prepared. The fucoidan content of this product is 72.5%
The recovery by weight and crude extract was 87.0%. Table 10 shows the results.

[0065]

[Table 10]

The absorbance at 520 nm of the 1% by weight solution of the product of the present invention is 0.05, it is 90% decolorized, it is slightly brown visually, and the flavor (odor and taste) peculiar to seaweed. Had been removed.

(2) Acetate ulcer healing promoting effect: Next, the acetic ulcer healing promoting effect of the product of the present invention was examined by the following method. That is, 8-week-old SD rats (body weight 250-3
The stomach was removed and 0.03 ml of 20% by weight acetic acid was added to the gastric body submucosa.
By injection, an acetic acid ulcer was formed in the rat, and the test sample was orally administered under the conditions shown in Table 11 for 5 days from the 5th to the 9th day after the ulcer occurred. 10 after administration
On the day, the stomach was excised and the area of the ulcer-forming part (major axis × minor axis) was measured, and this was used as the ulcer index to calculate the healing rate by the following formula. During the test period, food and water were freely available. Table 11 shows the results.

[0068]

Formula 2: Healing rate (%) = (1−C / D) × 100 C; ulcer index of fucoidan-administered group D; ulcer index of control group

[0069]

[Table 11]

As is clear from Table 11, the product of the present invention
Similar to the unbleached product obtained by purifying the crude purified extract, the anti-ulcer activity was not changed at all and retained a high healing promoting activity.

Test Example 2 Color tone test and sedimentation test: Toners of the present invention 1 and 2 and comparative products 1 and 2 were prepared according to a conventional method using Okinawa mozuku fucoidan having various decolorization rates shown in Table 12 below. did. The color tone and the sedimentation status of each lotion were evaluated by the following methods.

[0072]

[Table 12]

(Evaluation Method) In a random state in which each of the above lotions could not be specified, a visual evaluation was performed by a specialized panel of 10 persons. According to the evaluation criteria shown in Table 13, the color tone was evaluated according to the evaluation criteria shown in Table 13, and the average was calculated and determined.
Table 15 shows the results.

(Evaluation criteria)

[Table 13]

(Evaluation criteria)

[Table 14]

(Result)

[Table 15]

As shown in Table 15, in the color tone test, those with a decolorization rate of 0% and 50% showed annoying coloring, and were judged to have a considerably low commercial value in appearance. In contrast,
Those with a decolorization rate of 70% were determined to have little coloring and had almost sufficient commercial value, and those with 90% of the same were determined to have the least coloring and sufficient commercial value.

In the precipitation test, those having a decolorization rate of 0% and 50% showed noticeable precipitation and were judged to have a considerably low commercial value in appearance. On the other hand, those with a decoloration rate of 70% had little sedimentation and were judged to have almost sufficient commercial value, and those with 90% had the least sedimentation and were judged to have sufficient commercial value.

Example 1 Lotion: The following components were mixed by a conventional method to prepare a lotion.

(Ingredient) Compounding amount (% by weight) Ethanol 10 Glycerin 5 1,3-butylene glycol 5 Methylparaben 0.05 Polyoxyethylene hydrogenated castor oil 0.5 Carboxyvinyl polymer 0.1 Inventive fucoidan (*) 10 incense Material 0.05 Purified water balance *; Decolorization rate 97.0% (Experimental example 4, obtained with final ethanol concentration of 40% (V / V) and sodium chloride concentration of 10% by weight)

Example 2 Emulsion: The following components were mixed by a conventional method to produce an emulsion.

(Ingredient) Compounding amount (% by weight) Stearic acid 2 Cetanol 1 Vaseline 5 Liquid paraffin 10 Polyoxyethylene 2 Sorbitan monooleate Sorbitan monooleate 2 Butyl paraben 0.1 1,3-butylene glycol 5 Carboxymethyl cellulose 0.1 sodium hydroxide 0.05 methyl paraben 0.1 fucoidan (*) of the present invention 1 perfume 0.05 purified water balance *; decolorization rate 94.2% (Experimental example 5, carbohydrate concentration 2.90% by weight, (Final ethanol concentration of 45% (V / V), sodium chloride concentration of 10% by weight)

Example 3 Moisturizing cream: The following ingredients were mixed by a conventional method to produce a moisturizing cream.

(Ingredient) Compounding amount (% by weight) Stearic acid 4 Cetanol 2 Vaseline 5 Liquid paraffin 10 Polyoxyethylene 2 Sorbitan monostearate Sorbitan monostearate 3 Butylparaben 0.1 1,3-butylene glycol 2 Hydroxide Sodium 0.05 Fucoidan (*) of the present invention 0.01 Methyl paraben 0.1 Perfume 0.05 Purified water balance *; Decolorization rate 92.1% (Experimental example 6, carbohydrate concentration 5.0% by weight, final ethanol) At a concentration of 45% (V / V) and a concentration of 5% by weight of sodium chloride)

Example 4 Condyle Granules: The following formulation was mixed to prepare granules.

(Preparation) Compounding amount Fucoidan (*) of the present invention 0.5 g Dextrin 0.47 g Japanese Pharmacopoeia 0.03 g hydroxypropylcellulose 0.03 g *; Decolorization rate 90.7% (Experimental example 6, carbohydrate concentration 10.0 weight% %, Final ethanol concentration 40% (V / V), sodium chloride concentration 5% by weight)

[0087]

According to the present invention, high-purity fucoidan with reduced coloring substances and / or components causing seaweed odor can be efficiently produced. Further, the high-purity fucoidan of the present invention (for example, fucoidan derived from Okinawa mozuku)
Is pale and has no seaweed flavor. Therefore, it can be arbitrarily added to a wide range of foods and drinks, cosmetics, pharmaceuticals, etc. without impairing or deteriorating the original flavor of foods and drinks, cosmetics, pharmaceuticals, etc., and is useful for fucoidan. The effect can be utilized. that's all

──────────────────────────────────────────────────の Continued on the front page (51) Int.Cl. ⁷ Identification FI theme coat ゛ (Reference) A23L 1/337 A61K 31/725 (72) Inventor Shusuke Hashimoto 1-1-19 Higashi-Shimbashi, Minato-ku, Tokyo Yakult Honsha Co., Ltd. (72) Inventor Masato Nagaoka 1-119 Higashi-Shimbashi, Minato-ku, Tokyo Tokyo (72) Inventor Minoru Ichioka 1-1-19 Higashi-Shimbashi, Minato-ku, Tokyo Yakult Honsha (72) Inventor Yoshio Hiraki 1-1-19 Higashi-Shimbashi, Minato-ku, Tokyo Japan (72) Inventor Satoshi Yoshikawa 1-1-19, Higashi-Shimbashi, Minato-ku, Tokyo Yakult Honsha Co., Ltd. (72) Inventor Hiroshi Kono 1-1-19 Higashi-Shimbashi, Minato-ku, Tokyo Co., Ltd. Yakult Honsha Co., Ltd. (72) Inventor Masahiko Inami 5-Shizakizaki, Gushikawa-shi, Okinawa F-term (reference) in Tropical Techno Center Co., Ltd. 4B018 MD33 MD67 ME11 MF01 MF05 MF06 4B019 LC05 LP07 LP09 LP13 4C083 AB032 AC012 AC022 AC072 AC102 AC122 AC242 AC402 AC432 AC442 AC482 AD092 AD242 AD282 AD311 AD312 CC04 CC05 DD16 DD23 DD01 DD27 DD01 4C086 AA01 AA02 AA03 EA20 GA17 MA01 MA04 MA63 NA09 ZA68 ZA89 4C090 AA01 AA04 BA61 BC06 BD22 CA04 CA06 CA09 CA10 CA18 CA19 CA47 DA09 DA23 DA26

Claims (8)

[Claims] 1. The following steps a) and b): a) freezing and re-thawing a hot-water or acid extract of seaweed or drying and re-thawing; b) said re-thawing Alternatively, high-purity fucoidan produced by a method comprising a step of adding an alcohol to the re-dissolved hot water or acid extract of seaweed to remove a precipitate. 2. the following steps a) and c): a) freezing and re-thawing the hot-water or acid extract of seaweed or drying and re-thawing; c) said re-thawing Alternatively, high-purity fucoidan produced by a method comprising a step of adding an alcohol to the re-dissolved seaweed hot water or acid extract in the presence of a salt to remove a precipitate. 3. The high-purity fucoidan according to claim 1, wherein the seaweed is Okinawa mozuku and is substantially free of color. 4. The following steps a) and b): a) freezing and re-thawing the hot-water or acid extract of seaweed or drying and re-thawing; b) the re-thawing Alternatively, a method for producing high-purity fucoidan, comprising a step of adding an alcohol to hot water or an acid extract of the redissolved seaweed to remove a precipitate. 5. The following steps a) and c): a) freezing and re-thawing the hot-water or acid extract of seaweed or drying and re-thawing; c) said re-thawing Alternatively, a method for producing high-purity fucoidan, comprising a step of adding an alcohol to the re-dissolved hot water or acid extract of seaweed in the presence of a salt to remove a precipitate. 6. A medicament comprising the high-purity fucoidan according to any one of claims 1 to 3 as an active ingredient. 7. The method according to claim 6, which is a preventive or therapeutic agent for gastrointestinal ulcer.
The medicament according to claim. 8. A cosmetic comprising the high-purity fucoidan according to any one of claims 1 to 3.