WO2017164411A1 - Antitumor method or antitumor material using mixture of fucoidan with moromi vinegar - Google Patents

Antitumor method or antitumor material using mixture of fucoidan with moromi vinegar Download PDF

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WO2017164411A1
WO2017164411A1 PCT/JP2017/012202 JP2017012202W WO2017164411A1 WO 2017164411 A1 WO2017164411 A1 WO 2017164411A1 JP 2017012202 W JP2017012202 W JP 2017012202W WO 2017164411 A1 WO2017164411 A1 WO 2017164411A1
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fucoidan
moromi vinegar
moromi
vinegar
growth rate
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哲 渡嘉敷
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株式会社クレイ沖縄
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    • A—HUMAN NECESSITIES
    • A23—FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23L—FOODS, FOODSTUFFS, OR NON-ALCOHOLIC BEVERAGES, NOT COVERED BY SUBCLASSES A21D OR A23B-A23J; THEIR PREPARATION OR TREATMENT, e.g. COOKING, MODIFICATION OF NUTRITIVE QUALITIES, PHYSICAL TREATMENT; PRESERVATION OF FOODS OR FOODSTUFFS, IN GENERAL
    • A23L33/00—Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof
    • A23L33/10—Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof using additives
    • A23L33/105—Plant extracts, their artificial duplicates or their derivatives
    • A—HUMAN NECESSITIES
    • A23—FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23L—FOODS, FOODSTUFFS, OR NON-ALCOHOLIC BEVERAGES, NOT COVERED BY SUBCLASSES A21D OR A23B-A23J; THEIR PREPARATION OR TREATMENT, e.g. COOKING, MODIFICATION OF NUTRITIVE QUALITIES, PHYSICAL TREATMENT; PRESERVATION OF FOODS OR FOODSTUFFS, IN GENERAL
    • A23L33/00—Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof
    • A23L33/10—Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof using additives
    • A23L33/14—Yeasts or derivatives thereof
    • A23L33/145—Extracts
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K31/00—Medicinal preparations containing organic active ingredients
    • A61K31/33—Heterocyclic compounds
    • A61K31/335—Heterocyclic compounds having oxygen as the only ring hetero atom, e.g. fungichromin
    • A61K31/336—Heterocyclic compounds having oxygen as the only ring hetero atom, e.g. fungichromin having three-membered rings, e.g. oxirane, fumagillin
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61K—PREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K31/00—Medicinal preparations containing organic active ingredients
    • A61K31/70—Carbohydrates; Sugars; Derivatives thereof
    • A61K31/715—Polysaccharides, i.e. having more than five saccharide radicals attached to each other by glycosidic linkages; Derivatives thereof, e.g. ethers, esters
    • A61K31/737—Sulfated polysaccharides, e.g. chondroitin sulfate, dermatan sulfate
    • 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
    • A61K36/02—Algae
    • A61K36/03—Phaeophycota or phaeophyta (brown algae), e.g. Fucus
    • 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)
    • A61K36/88—Liliopsida (monocotyledons)
    • A61K36/899—Poaceae or Gramineae (Grass family), e.g. bamboo, corn or sugar cane

Definitions

  • the present invention relates to an invention in which fucoidan such as acetyl fucoidan can be reduced by using a method or substance for mixing fucoidan and moromi vinegar, and cheap moromi vinegar can be substituted.
  • fucoidan such as acetyl fucoidan
  • mozuku is the main component, and moromi vinegar and brown sugar and appropriate drinking water are added to this as well.
  • a health food drink which is prepared by mixing and heating with stirring, and simultaneously applying an AC voltage for a certain period of time with an electrostatic induction device to refine the molecules of the above solution by electrostatic induction and then sterilizing. Is known.
  • mozuku extract that is, fucoidan
  • an electromagnetic alternating magnetic field is simultaneously applied to moromi vinegar and mozuku, and electrons, atoms
  • fucoidan has a molecular weight that is easily absorbed by the body through the action at the molecular level.
  • acetylfucoidan is considered promising as a pharmaceutical composition for oral administration for treating malignant tumors that develop in the digestive tract.
  • acetyl fucoidan is very expensive, it is difficult to put it to practical use for economic reasons.
  • the technical problem of the present invention has been focused on such problems, and has found that the proliferation rate of tumor cells can be further suppressed by mixing and administering inexpensive moromi vinegar.
  • the present inventors unexpectedly compared the solution added with only acetylfucoidan or moromi vinegar and the solution added with the mixture of both in comparison with the antitumor activity of the mixture added alone. It was found that the rate of decrease was high. And further examination was repeated and it came to complete this invention.
  • a pharmaceutical composition for tumor treatment containing fucoidan and moromi vinegar containing fucoidan and moromi vinegar.
  • a pharmaceutical composition that suppresses the growth rate of tumor cells containing fucoidan and moromi vinegar containing fucoidan and moromi vinegar.
  • the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, (1) or (2) A pharmaceutical composition according to 1.
  • a tumor cell growth rate suppressor characterized by suppressing the growth rate of tumor cells with a substance obtained by mixing fucoidan separated from seaweed and moromi vinegar.
  • the moromi vinegar content is 3% to 95%, and the fucoidan is derived from seaweeds such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, hondaidae, It is a method for suppressing the growth rate of tumor cells described in 7).
  • the amount of the moromi vinegar is 3% to 95%, and the fucoidan is derived from seaweed such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, (8) It is the described tumor cell growth rate inhibitor.
  • the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, (7) or (9) This is a method for suppressing the growth rate of tumor cells.
  • the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, described in (8) or (10) It is a substance that suppresses the growth rate of tumor cells.
  • the pharmaceutical composition containing fucoidan and moromi vinegar according to the present invention ((1) to (6) has an effect of suppressing the growth rate of tumor cells, and can be replaced by cheap moromi vinegar by reducing the amount of fucoidan used. Since various types of fucoidan are sufficient instead of acetylfucoidan, various seaweeds can be used, especially when acetylfucoidan separated from Okinawa mozuku and moromi vinegar are mixed together to reduce expensive acetylfucoidan and reduce moromi vinegar. In addition, fucoidan and moromi vinegar have no toxicity, so there are no side effects like conventional chemotherapeutic agents, reducing the burden of side effects on patients.
  • the result of the experiment is that the amount of fucoidan used can be reduced and cheap moromi vinegar can be substituted found. Since various types of fucoidan are sufficient instead of acetyl fucoidan, various seaweeds can be used. In particular, when acetyl fucoidan separated from Okinawa mozuku and moromi vinegar are mixed, there is an effect that expensive acetyl fucoidan can be reduced and cheap moromi vinegar can be substituted.
  • the moromi vinegar content is 3% to 95%
  • the fucoidan is derived from seaweeds such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, hondawali, etc. Vinegar is widely used, and fucoidan can be collected from seaweeds other than Okinawa mozuku.
  • the blended amount of moromi vinegar is 3% to 95%
  • the fucoidan is derived from seaweed such as mozuku, wakame, mekabu, kombu, hijiki, akamoku. It is wide and fucoidan can be collected and used from seaweeds other than Okinawa mozuku.
  • the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi vinegar,
  • the range of adoption is large and various raw materials can be adopted.
  • the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi vinegar,
  • the range of adoption is large and various raw materials can be adopted.
  • FIG. 4 is a flowchart illustrating a mixing method according to the present invention.
  • Fucoidan (English name: fucoidan) is a kind of sulfated polysaccharide. It is a dietary fiber that is abundant in mucilage of brown algae such as kombu, wakame (including mekabu which is partly), and mozuku. L-fucose (polysaccharide) is a compound in which dozens to hundreds of thousands are linked by ⁇ 1-2 and ⁇ 1-4 bonds, and the average molecular weight is about 200,000. It is classified into U-fucoidan containing glucuronic acid, F-fucoidan consisting only of sulfated fucose, and G-fucoidan containing galactose. Fucoidan is a generic name, and a portion of moromi vinegar stock powder is acetyl fucoidan. In the present invention, fucoidan powder purchased from Kinshu Bio Co., Ltd. was used.
  • Moromi vinegar is a liquid obtained by compression-filtering moromi koji produced in the manufacturing process of “Awamori”, a distilled liquor from Okinawa (Ryukyu Islands). Although it is called moromi vinegar, it contains almost no acetic acid and is a soft drink rich in amino acids and citric acid. In the present invention, a powdered moromi vinegar stock solution purchased from Niisato Sake Brewery was used.
  • the pharmaceutical composition of the present invention can be produced by mixing a concentrated powder or an undiluted solution produced from a stock solution of moromi vinegar with fucoidan powder.
  • the ratio of fucoidan and moromi vinegar can be adjusted to maximize the effect of suppressing the growth rate of tumor cells.
  • the ratio of fucoidan and moromi vinegar is 1 to 9 parts by weight, preferably 1 to 3 parts by weight, and more preferably 1 part by weight with respect to 1 part by weight of fucoidan.
  • the pharmaceutical composition of the present invention is preferably a pharmaceutical composition for oral administration.
  • the pharmaceutical composition for oral administration of the present invention may be a powder, a kneaded product, a tablet liquid or a tablet, preferably a powder, a kneaded product or a tablet.
  • the solid preparation of the present invention is preferably further encapsulated or subjected to a coating treatment on the surface. Encapsulated preparations and coating preparations can be produced using known methods.
  • the yield of acetylfucoidan is as follows.
  • the yield of acetyl fucoidan isolated from Okinawa mozuku is shown in Table 1. 2.3% crude polysaccharide was obtained from wet algal cells. When this crude polysaccharide was purified, a purified polysaccharide was obtained in a yield of 2.0%. These numbers were higher than the previous results.
  • Okinawa Mozuku contains only a small amount of alginic acid (1/10), and most of the macromolecules contained in algal cells can be called acetylfucoidan.
  • acetyl fucoidan The yield of acetyl fucoidan is shown in Table 1.
  • Table 2 shows the results of analyzing the total sugar, uronic acid and sulfuric acid contents of acetyl fucoidan by the phenol sulfuric acid, carbazole sulfuric acid and gelatin suspension methods.
  • the total sugar, D-glucuronic acid and sulfuric acid contents of this polysaccharide were 66.9%, 14.1% and 15.8%, respectively.
  • the components of acetyl fucoidan are as follows.
  • Table 2 shows the chemical structure of acetylfucoidan.
  • Acetylfucoidan is hydrolyzed with 2.0 M sulfuric acid (100 ° C, 2 hours), neutralized with barium carbonate, concentrated, and separated and identified by high-performance liquid chromatograph (DX500: Dionex). went. L-fucose and D-xylose were identified from the liquid chromatogram. It can be seen that most are polysaccharides composed of L-fucose.
  • Table 3 shows the growth inhibitory effect of acetylfucoidan on U937 cells.
  • the measured value of the culture solution of U937 cells to which only distilled water was added was defined as 100 (control), and the percentage relative thereto was displayed.
  • Preliminary experiments on the amount of addition were performed, and this experiment was performed under the following conditions (three types).
  • When only 500 ⁇ g of acetyl fucoidan was added the proliferation rate of tumor cells was reduced to 80%.
  • moromi vinegar was added, it decreased to 90%.
  • the growth rate of the culture solution in which both were mixed decreased to 71%, and a significant synergistic effect was observed.

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Abstract

[Problem] To realize a technique whereby the proliferation rate of tumor cells can be more decreased by administering a mixture comprising less expensive moromi (sake mash) vinegar. [Solution] The proliferation rate of tumor cells is decreased by using a material comprising a mixture of marine alga-derived fucoidan and moromi vinegar. In particular, by using a mixture of acetyl fucoidan separated from Cladosiphon okamuranus Tokida with moromi vinegar, the less expensive moromi vinegar can substitute for the acetyl fucoidan and thus an effect of reducing the amount of the expensive acetyl fucoidan to be used can be achieved. The moromi vinegar as described above is used in an amount of 3-95%. The fucoidan as described above is derived from a marine alga such as Nemacystus decipiens, Undaria pinnatifida, Undaria pinnatifida sporophyll, Laminariaceae algae, Sargassum fusiforme, Sargassum horneri (Turner) C. Agardh or a marine alga belonging to the family Sargassaceae.

Description

フコイダンともろみ酢とを混合した抗腫瘍方法又は物質Anti-tumor method or substance mixed with fucoidan and moromi vinegar
　本発明は、フコイダンともろみ酢とを混合する方法又は物質により、高価なアセチルフコイダンなどのフコイダンを減らして安価なもろみ酢で代用できる発明に関する。 The present invention relates to an invention in which fucoidan such as acetyl fucoidan can be reduced by using a method or substance for mixing fucoidan and moromi vinegar, and cheap moromi vinegar can be substituted.
　特許文献１のように、飲み易いものであると共に、体内で吸収し易いもずくエキス入りの健康食品飲料を提供するべく、もずくを主成分とし、これにもろみ酢及び黒糖及び適宜の飲料水を加えて混ぜ合わせ、攪拌加熱処理すると同時に、これを静電誘導装置により、一定時間交流電圧を印加し、静電誘導作用により上記の溶液の分子を微細化し、その後殺菌処理して成る、健康食品飲料は知られている。もずくのエキス、即ちフコイダンを抽出するに際し、静電誘導反応装置を用いて交流高圧電界による静電誘導作用に加えて、電磁気的な交流磁場を同時にもろみ酢、及びもずくに作用させ、電子、原子、分子レベルでの作用を通じて、フコイダンを体内吸収し易い分子量にした発明も知られている。 In order to provide a health food drink containing mozuku extract that is easy to drink and absorbs easily in the body as in Patent Document 1, mozuku is the main component, and moromi vinegar and brown sugar and appropriate drinking water are added to this as well. A health food drink, which is prepared by mixing and heating with stirring, and simultaneously applying an AC voltage for a certain period of time with an electrostatic induction device to refine the molecules of the above solution by electrostatic induction and then sterilizing. Is known. In extracting mozuku extract, that is, fucoidan, in addition to electrostatic induction action by an alternating high voltage electric field using an electrostatic induction reaction device, an electromagnetic alternating magnetic field is simultaneously applied to moromi vinegar and mozuku, and electrons, atoms There is also known an invention in which fucoidan has a molecular weight that is easily absorbed by the body through the action at the molecular level.
　また、特許文献２のように、アセチルフコイダンを有効成分とする消化管に発症した悪性腫瘍を治療するための経口投与用医薬組成物を提供することを目的に、養殖オキナワモズクを原料として製造されたアセチルフコイダンを水に溶かして経口投与することによって、マウス大腸癌由来の細胞ｃｅｌｌｌｉｎｅであるＣｏｌｏｎ２６細胞を腸に移植して大腸がんを発症させたマウスの、体重減少と悪性腫瘍の重量の増大を有意（Ｐ＝０．０５）に減少させた。 In addition, as disclosed in Patent Document 2, for the purpose of providing a pharmaceutical composition for oral administration for treating a malignant tumor that has developed in the gastrointestinal tract containing acetylfucoidan as an active ingredient, it is produced using cultured Okinawa mozuku as a raw material. Acetylfucoidan dissolved in water and orally administered, colon 26 cells, which are cell lines derived from mouse colon cancer, were transplanted into the intestine, resulting in colon cancer and weight loss and increased malignant tumor weight Was significantly reduced (P = 0.05).
特開2008-22787号公報JP 2008-22787 特開平2009-185009 公報Japanese Unexamined Patent Publication No. 2009-185009
　ところが、特許文献２のように、アセチルフコイダンが消化管に発症した悪性腫瘍を治療するための経口投与用医薬組成物として有望視されている。しかしながら、アセチルフコイダンは極めて高価なため、経済的な理由で実用化が困難と成っている。
　本発明の技術的課題は、このような問題に着目し、安価なもろみ酢を混合して投与することで、腫瘍細胞の増殖率をより抑制できることを究明した。 However, as in Patent Document 2, acetylfucoidan is considered promising as a pharmaceutical composition for oral administration for treating malignant tumors that develop in the digestive tract. However, since acetyl fucoidan is very expensive, it is difficult to put it to practical use for economic reasons.
The technical problem of the present invention has been focused on such problems, and has found that the proliferation rate of tumor cells can be further suppressed by mixing and administering inexpensive moromi vinegar.
　本発明者は、アセチルフコイダン、またはもろみ酢のみを添加した溶液と両者の混合液を添加した溶液を比較すると、両者の混合液の抗腫瘍活性が単独で添加したものに比較して予想外に高い減少率を示したことを見出した。そして、更に検討を重ね、本発明を完成するに到った。 The present inventors unexpectedly compared the solution added with only acetylfucoidan or moromi vinegar and the solution added with the mixture of both in comparison with the antitumor activity of the mixture added alone. It was found that the rate of decrease was high. And further examination was repeated and it came to complete this invention.
　すなわち、本発明は、下記記載の発明を提供することにより、上記課題を解決したものである。
（１）フコイダンともろみ酢を含有する腫瘍治療用医薬組成物。
（２）フコイダンともろみ酢を含有する腫瘍細胞の増殖率を抑制する医薬組成物。
（３）前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク及び/又はホンダワラ科の海藻を由来としていることを特徴とする、（１）又は（２）に記載の医薬組成物。
（４）前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末であることを特徴とする、請求項（１）又は（２）に記載の医薬組成物。
（５）フコイダンともろみ酢の比率が、フコイダン１重量部に対し、もろみ酢が１～９重量部であることを特徴とする、（１）～（４）のいずれか１項に記載の医薬組成物。
（６）フコイダンは、アセチルフコイダンである、（１）～（５）のいずれか１項に記載の医薬組成物。
（７）海藻から分離したフコイダンともろみ酢とを混合した物質により腫瘍細胞の増殖率を抑制することを特徴とする腫瘍細胞の増殖率を抑制する方法である。特に、オキナワモズクから分離したアセチルフコイダンともろみ酢とを混合すると、高価なアセチルフコイダンを減らして安価なもろみ酢で代用できる効果が有る。
（８）海藻から分離したフコイダンともろみ酢とを混合した物質により腫瘍細胞の増殖率を抑制することを特徴とする腫瘍細胞の増殖率抑制物質である。
（９）前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク、ホンダワラ科などの海藻を由来としていることを特徴とする、（７）に記載の腫瘍細胞の増殖率を抑制する方法である。
（１０）前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモクなどの海藻を由来としていることを特徴とする、（８）に記載の腫瘍細胞の増殖率抑制物質である。
（１１）前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末であることを特徴とする、（７）又は（９）に記載の腫瘍細胞の増殖率を抑制する方法である。
（１２）前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末であることを特徴とする、（８）又は（１０）に記載の腫瘍細胞の増殖率抑制物質である。 That is, this invention solves the said subject by providing the invention of the following description.
(1) A pharmaceutical composition for tumor treatment containing fucoidan and moromi vinegar.
(2) A pharmaceutical composition that suppresses the growth rate of tumor cells containing fucoidan and moromi vinegar.
(3) The pharmaceutical composition according to (1) or (2), wherein the fucoidan is derived from mozuku, wakame, mekabu, kombu, hijiki, akamoku, and / or a seaweed of the genus Honda.
(4) The moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, (1) or (2) A pharmaceutical composition according to 1.
(5) The pharmaceutical according to any one of (1) to (4), wherein the ratio of fucoidan and moromi vinegar is 1 to 9 parts by weight of moromi vinegar to 1 part by weight of fucoidan. Composition.
(6) The pharmaceutical composition according to any one of (1) to (5), wherein the fucoidan is acetyl fucoidan.
(7) A method for suppressing the growth rate of tumor cells, wherein the growth rate of tumor cells is suppressed by a substance obtained by mixing fucoidan separated from seaweed and moromi vinegar. In particular, when acetyl fucoidan separated from Okinawa mozuku and moromi vinegar are mixed, there is an effect that expensive acetyl fucoidan can be reduced and cheap moromi vinegar can be substituted.
(8) A tumor cell growth rate suppressor characterized by suppressing the growth rate of tumor cells with a substance obtained by mixing fucoidan separated from seaweed and moromi vinegar.
(9) The moromi vinegar content is 3% to 95%, and the fucoidan is derived from seaweeds such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, hondaidae, It is a method for suppressing the growth rate of tumor cells described in 7).
(10) The amount of the moromi vinegar is 3% to 95%, and the fucoidan is derived from seaweed such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, (8) It is the described tumor cell growth rate inhibitor.
(11) The moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, (7) or (9) This is a method for suppressing the growth rate of tumor cells.
(12) The moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, described in (8) or (10) It is a substance that suppresses the growth rate of tumor cells.
　本発明のフコイダンともろみ酢を含有する医薬組成物（（１）～（６）は、腫瘍細胞の増殖率を抑制する効果を奏し、フコイダンの使用量を減らして安価なもろみ酢で代用できること判明した。アセチルフコイダンでなく、多種のフコイダンでも足りるので、各種の海藻を使用できる。特に、オキナワモズクから分離したアセチルフコイダンともろみ酢とを混合すると、高価なアセチルフコイダンを減らして安価なもろみ酢で代用できる効果が有る。また、フコイダンともろみ酢の毒性は認められないので、従来の化学療法剤のような副作用はなく、患者の副作用の負担を軽減できる。さらに安価なもろみ酢を原料とするので、大量養殖が可能であり、安価に製造できる。
　（７）のように、海藻から分離したフコイダンともろみ酢とを混合した物質により腫瘍細胞の増殖率を抑制する方法によると実験の結果、フコイダンの使用量を減らして安価なもろみ酢で代用できること判明した。アセチルフコイダンでなく、多種のフコイダンでも足りるので、各種の海藻を使用できる。特に、オキナワモズクから分離したアセチルフコイダンともろみ酢とを混合すると、高価なアセチルフコイダンを減らして安価なもろみ酢で代用できる効果が有る。 The pharmaceutical composition containing fucoidan and moromi vinegar according to the present invention ((1) to (6) has an effect of suppressing the growth rate of tumor cells, and can be replaced by cheap moromi vinegar by reducing the amount of fucoidan used. Since various types of fucoidan are sufficient instead of acetylfucoidan, various seaweeds can be used, especially when acetylfucoidan separated from Okinawa mozuku and moromi vinegar are mixed together to reduce expensive acetylfucoidan and reduce moromi vinegar. In addition, fucoidan and moromi vinegar have no toxicity, so there are no side effects like conventional chemotherapeutic agents, reducing the burden of side effects on patients. Therefore, it can be mass-cultured and manufactured at low cost.
(7) According to the method to suppress the growth rate of tumor cells with a substance mixed with fucoidan separated from seaweed and moromi vinegar, the result of the experiment is that the amount of fucoidan used can be reduced and cheap moromi vinegar can be substituted found. Since various types of fucoidan are sufficient instead of acetyl fucoidan, various seaweeds can be used. In particular, when acetyl fucoidan separated from Okinawa mozuku and moromi vinegar are mixed, there is an effect that expensive acetyl fucoidan can be reduced and cheap moromi vinegar can be substituted.
　（８）のように、海藻から分離したフコイダンともろみ酢とを混合した物質によると実験の結果、フコイダンの使用量を減らして安価なもろみ酢で代用できること判明した。 As shown in (8), according to the substance mixed with fucoidan and moromi vinegar separated from seaweed, it was found as a result of the experiment that the amount of fucoidan used can be reduced and cheap moromi vinegar can be substituted.
　（９）のように、前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク、ホンダワラ科などの海藻を由来としているので、もろみ酢の使用幅が大きく、またフコイダンは、オキナワモズク以外の海藻からも採取して使用できる。 As in (9), the moromi vinegar content is 3% to 95%, and the fucoidan is derived from seaweeds such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, hondawali, etc. Vinegar is widely used, and fucoidan can be collected from seaweeds other than Okinawa mozuku.
　（１０）のように、前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモクなどの海藻を由来としているので、もろみ酢の使用幅が大きく、またフコイダンは、オキナワモズク以外の海藻からも採取して使用できる。 As in (10), the blended amount of moromi vinegar is 3% to 95%, and the fucoidan is derived from seaweed such as mozuku, wakame, mekabu, kombu, hijiki, akamoku. It is wide and fucoidan can be collected and used from seaweeds other than Okinawa mozuku.
　（１１）のように、前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末及び／又はもろみ粕であるので、もろみ酢としての採択幅が大きく、原料も種々採択できる。 As in (11), the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi vinegar, The range of adoption is large and various raw materials can be adopted.
　（１２）のように、前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末及び／又はもろみ粕であるので、もろみ酢としての採択幅が大きく、原料も種々採択できる。 As in (12), the moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi vinegar, The range of adoption is large and various raw materials can be adopted.
本発明による混合方法を示すフローチャートである。4 is a flowchart illustrating a mixing method according to the present invention.
　特に言及しない限り、本明細書及び特許請求の範囲で用いた用語は以下に述べる意味を有する。 Unless otherwise stated, the terms used in this specification and claims have the meanings described below.
フコイダン
　フコイダン（英語名：fucoidan）は、硫酸化多糖の一種である。コンブやワカメ（一部位であるメカブを含む）、、 モズクなど褐藻類の粘質物に多く含まれる食物繊維である。主に L-フコース（多糖体）が α1-2、α1-4結合で数十から数十万個も繋がった化合物で、平均分子量は約200,000。グルクロン酸を含む U-フコイダン、硫酸化フコースだけからなる F-フコイダン、ガラクトースを含むG-フコイダンなどに分類される。フコイダンとは総称であって、もろみ酢原液粉末その一部がアセチルフコイダンである。本発明では、金秀バイオ株式会社から購入したフコイダン粉末を用いた。 Fucoidan (English name: fucoidan) is a kind of sulfated polysaccharide. It is a dietary fiber that is abundant in mucilage of brown algae such as kombu, wakame (including mekabu which is partly), and mozuku. L-fucose (polysaccharide) is a compound in which dozens to hundreds of thousands are linked by α1-2 and α1-4 bonds, and the average molecular weight is about 200,000. It is classified into U-fucoidan containing glucuronic acid, F-fucoidan consisting only of sulfated fucose, and G-fucoidan containing galactose. Fucoidan is a generic name, and a portion of moromi vinegar stock powder is acetyl fucoidan. In the present invention, fucoidan powder purchased from Kinshu Bio Co., Ltd. was used.
もろみ酢
　もろみ酢とは、沖縄（琉球諸島）産蒸留酒である「泡盛」の製造過程で生じたもろみ粕を圧縮濾過した液体のことである。もろみ酢と称されているが、酢酸はほとんど含まれておらず、アミノ酸とクエン酸が豊富な清涼飲料水である。本発明では、合名会社新里酒造から購入したもろみ酢原液を粉末にしたものを用いた。 Moromi vinegar Moromi vinegar is a liquid obtained by compression-filtering moromi koji produced in the manufacturing process of “Awamori”, a distilled liquor from Okinawa (Ryukyu Islands). Although it is called moromi vinegar, it contains almost no acetic acid and is a soft drink rich in amino acids and citric acid. In the present invention, a powdered moromi vinegar stock solution purchased from Niisato Sake Brewery was used.
フコイダンともろみ酢を含有する医薬組成物
　本発明の医薬組成物は、もろみ酢の原液から製造した濃縮粉末又は原液をフコイダンの粉末と混ぜ合わせて、製造することができる。フコイダンともろみ酢の比率は、腫瘍細胞の増殖率抑制効果を最大に発揮できるように調整することができる。フコイダンともろみ酢の比率が、フコイダン１重量部に対し、もろみ酢が１～９重量部であり、好ましくは、１～３重量部であり、より好ましくは、１重量部である。本発明の医薬組成物は、好ましく経口投与用医薬組成物である。また本発明の経口投与用医薬組成物は、粉末、練り物、錠剤液体又はであってもよく、好ましくは、粉末、練り物、又は錠剤である。本発明の固形製剤は、更にカプセル化されるか、表面にコーティング処理が施されることが好ましい。カプセル化製剤やコーティング製剤は公知の方法を利用して製造できる。 Pharmaceutical Composition Containing Fucoidan and Moromi Vinegar The pharmaceutical composition of the present invention can be produced by mixing a concentrated powder or an undiluted solution produced from a stock solution of moromi vinegar with fucoidan powder. The ratio of fucoidan and moromi vinegar can be adjusted to maximize the effect of suppressing the growth rate of tumor cells. The ratio of fucoidan and moromi vinegar is 1 to 9 parts by weight, preferably 1 to 3 parts by weight, and more preferably 1 part by weight with respect to 1 part by weight of fucoidan. The pharmaceutical composition of the present invention is preferably a pharmaceutical composition for oral administration. The pharmaceutical composition for oral administration of the present invention may be a powder, a kneaded product, a tablet liquid or a tablet, preferably a powder, a kneaded product or a tablet. The solid preparation of the present invention is preferably further encapsulated or subjected to a coating treatment on the surface. Encapsulated preparations and coating preparations can be produced using known methods.
　次に、オキナワモズク由来のアセチルフコイダンともろみ酢とを混合した結果の抗腫瘍効果を詳述する。実験の結果、アセチルフコイダンの収率は次のとおりである。オキナワモズクから分離したアセチルフコイダンの収率を表１に示した。湿潤藻体から2.3%の粗多糖を得た。この粗多糖を精製すると2.0%の収率で精製多糖を得た。これらの数字は従来の結果と比較して多い結果となった。しかしながら。オキナワモズクにはわずかのアルギン酸（1/10）が含まれるのみで、藻体中に含まれる高分子はほとんどがアセチルフコイダンと言って良い。 Next, the antitumor effect resulting from mixing acetylfucoidan derived from Okinawa mozuku and moromi vinegar will be described in detail. As a result of the experiment, the yield of acetylfucoidan is as follows. The yield of acetyl fucoidan isolated from Okinawa mozuku is shown in Table 1. 2.3% crude polysaccharide was obtained from wet algal cells. When this crude polysaccharide was purified, a purified polysaccharide was obtained in a yield of 2.0%. These numbers were higher than the previous results. However. Okinawa Mozuku contains only a small amount of alginic acid (1/10), and most of the macromolecules contained in algal cells can be called acetylfucoidan.
　従って、一般的に藻体から抽出出来るのはオキナワモズクに存在するアセチルフコイダンの35％に留まる。他の褐藻類（コンブ、ワカメおよびヒジキ：これらのフコイダンの含量はアルギン酸の1/3 ）と比較すると、オキナワモズクは極めて高い含有のフコイダンを含む事が分かる。フコイダンの含有量の視点から見ると、オキナワモズクは極めて特異な海藻である事がわかる。 Therefore, in general, only 35% of acetylfucoidan present in Okinawa mozuku can be extracted from algal cells. Compared with other brown algae (comb, seaweed and hydrangea: these fucoidan content is 1/3 of that of alginic acid), Okinawa mozuku shows very high fucoidan content. From the viewpoint of fucoidan content, Okinawa Mozuku is a very unique seaweed.
　また、オキナワモズクの生育の北限が鹿児島県の奄美地方で、南限が沖縄県の石垣島である。これらの特性から、オキナワモズクは沖縄県が世界に誇る生物資源である事が理解できる。
アセチルフコイダンの収率を表１に示す。
Figure JPOXMLDOC01-appb-T000001
 　アセチルフコイダンの全糖、ウロン酸および硫酸含量をフェノール硫酸、カルバゾール硫酸およびゼラチン懸濁法で分析した結果を表２に示した。本多糖の全糖、Ｄ- グルクロン酸および硫酸含量は、それぞれ66.9% 、14.1% および15.8％であった。
アセチルフコイダンの構成成分は次のとおりである。
　アセチルフコイダンの化学構成を表２に示す。
Figure JPOXMLDOC01-appb-T000002
 　アセチルフコイダンを2.0 Ｍの硫酸で加水分解（100 ℃、2 時間）を行い、炭酸バリウムで中和した後、濃縮して高速液体クロマトグラフ（ＤＸ500 ：ダイオネックス社）で構成糖の分離・同定を行った。液体クロマトグラムから、Ｌ- フコースとＤ- キシロースを同定した。ほとんどがＬ- フコースで構成される多糖である事が分かる。 The northern limit of Okinawa mozuku grows in the Amami region of Kagoshima Prefecture, and the southern limit is Ishigaki Island in Okinawa Prefecture. From these characteristics, Okinawa Mozuku can be understood to be the world's proud biological resources.
The yield of acetyl fucoidan is shown in Table 1.
Figure JPOXMLDOC01-appb-T000001
 Table 2 shows the results of analyzing the total sugar, uronic acid and sulfuric acid contents of acetyl fucoidan by the phenol sulfuric acid, carbazole sulfuric acid and gelatin suspension methods. The total sugar, D-glucuronic acid and sulfuric acid contents of this polysaccharide were 66.9%, 14.1% and 15.8%, respectively.
The components of acetyl fucoidan are as follows.
Table 2 shows the chemical structure of acetylfucoidan.
Figure JPOXMLDOC01-appb-T000002
 Acetylfucoidan is hydrolyzed with 2.0 M sulfuric acid (100 ° C, 2 hours), neutralized with barium carbonate, concentrated, and separated and identified by high-performance liquid chromatograph (DX500: Dionex). went. L-fucose and D-xylose were identified from the liquid chromatogram. It can be seen that most are polysaccharides composed of L-fucose.
　この結果と他の化学分析の結果から、フコイダンの構成成分とその比は、Ｌ- フコース：Ｄ- キシロース：Ｄ- グルクロン酸：酢酸：硫酸＝4.0 ：0.1 ：1.0 ：1.0 ：1.0 であった。1996～7 年に、酢酸基を置換するフコイダンはオキナワモズクのみであった。この点からみても極めて特異なフコイダンであることがわかる。また、他のモズク、コンブおよびヒジキには高い含量の硫酸基が存在（30～35％）する。構成糖も多様で、オキナワモズクに含まれる構成糖の他に、Ｄ- ガラクトースやＤ- グルコースなどを含む事が知られている。 From this result and the results of other chemical analyses, the constituents of fucoidan and the ratio thereof were L- fucose: D- xylose: D- glucuronic acid: acetic acid: sulfuric acid = 4.0: 0.1: 1.0: 1.0: 1.0. From 1996 to 2007, Okinawa mozuku was the only fucoidan replacing the acetate group. It can be seen from this point that it is a very unique fucoidan. In addition, other mozuku, kombu and hinoki have a high content of sulfate groups (30-35%). There are various constituent sugars, and it is known to contain D- 含 む galactose, D- glucose and the like in addition to the constituent sugars contained in Okinawa Mozuku.
　アセチルフコイダンの抗腫瘍活について：アセチルフコイダンのＵ937 細胞に対する増殖抑制効果を表３に示した。蒸留水のみを添加したＵ937 細胞の培養液の測定値を100 （コントロール）としてそれに対する％を表示した。添加量の予備実験を行い、下記の条件（３種類）で本実験を行った。
　アセチルフコイダンのみ５００μg を添加した場合、腫瘍細胞の増殖率は80％に減少した。もろみ酢のみを添加すると、90％に減少した。両者を混合（250 ＋250 μg ）した培養液の増殖率は71％に減少し、有意に相乗効果が認められた。また、アセチルフコイダンおよびもろみ酢の添加量を２倍（総濃度1000μg/ml）に増大すると、腫瘍細胞の増殖率はそれぞれ70％、85％および55％となった。さらに、添加総量を2000μg に増やすと、増殖率は65％、78％および45％に減少した。同様の実験を３回行ったがほとんど同様の結果を得た。
　アセチルフコイダンおよびもろみ酢添加による腫瘍細胞の増殖率（蒸留水のみ添加を100 ％）を表３に示す。
Figure JPOXMLDOC01-appb-T000003
 Antitumor activity of acetylfucoidan: Table 3 shows the growth inhibitory effect of acetylfucoidan on U937 cells. The measured value of the culture solution of U937 cells to which only distilled water was added was defined as 100 (control), and the percentage relative thereto was displayed. Preliminary experiments on the amount of addition were performed, and this experiment was performed under the following conditions (three types).
When only 500 μg of acetyl fucoidan was added, the proliferation rate of tumor cells was reduced to 80%. When only moromi vinegar was added, it decreased to 90%. The growth rate of the culture solution in which both were mixed (250 + 250 μg) decreased to 71%, and a significant synergistic effect was observed. Further, when the addition amount of acetyl fucoidan and moromi vinegar was doubled (total concentration 1000 μg / ml), the growth rate of tumor cells became 70%, 85% and 55%, respectively. Furthermore, when the total amount added was increased to 2000 μg, the growth rate decreased to 65%, 78% and 45%. Similar experiments were performed three times, but almost the same results were obtained.
Table 3 shows the growth rate of tumor cells by adding acetylfucoidan and moromi vinegar (100% addition of distilled water only).
Figure JPOXMLDOC01-appb-T000003
　アセチルフコイダン、またはもろみ酢のみを添加した溶液と両者の混合液を添加した溶液を比較すると、両者の混合液の抗腫瘍活性が単独で添加したものに比較して高い減少率を示し、明らかな相乗効果が認められた。 Comparing the solution containing only acetylfucoidan or moromi vinegar and the solution containing both, the antitumor activity of both solutions showed a high decrease rate compared to the one added alone, which is clear A synergistic effect was observed.
　オキナワモズクから分離したアセチルフコイダンともろみ酢とを混合した物質を投与すると、腫瘍細胞の増殖率を抑制することができた。しかも、もろみ酢はアセチルフコイダンに比べると、安価なため、入手が容易で実用化が期待できる。 When a substance mixed with acetylfucoidan and moromi vinegar separated from Okinawa mozuku was administered, the growth rate of tumor cells could be suppressed. Moreover, moromi vinegar is less expensive than acetyl fucoidan, so it can be easily obtained and put to practical use.
　１　アセチルフコイダン
　２　もろみ酢
　３　混合物
 
  1 Acetyl Fucoidan 2 Moromi Vinegar 3 Mixture

Claims (12)

  1. フコイダンともろみ酢を含有する腫瘍治療用医薬組成物。 A pharmaceutical composition for treating tumors comprising fucoidan and moromi vinegar.
  2. フコイダンともろみ酢を含有する腫瘍細胞の増殖率を抑制する医薬組成物。 A pharmaceutical composition that suppresses the growth rate of tumor cells containing fucoidan and moromi vinegar.
  3. 前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク及び/又はホンダワラ科の海藻を由来としていることを特徴とする、請求項１又は２に記載の医薬組成物。 3. The pharmaceutical composition according to claim 1 or 2, wherein the fucoidan is derived from mozuku, wakame, mekabu, kombu, hijiki, akamoku, and / or a seaweed of the kingfisher family.
  4. 前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末であることを特徴とする、請求項１又は２に記載の医薬組成物。 The said moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder, The pharmaceutical composition according to claim 1 or 2 characterized by things.
  5. フコイダンともろみ酢の比率が、フコイダン１重量部に対し、もろみ酢が１～９重量部であることを特徴とする、請求項１～４のいずれか１項に記載の医薬組成物。 The pharmaceutical composition according to any one of claims 1 to 4, wherein the ratio of fucoidan and moromi vinegar is 1 to 9 parts by weight of moromi vinegar to 1 part by weight of fucoidan.
  6. フコイダンは、アセチルフコイダンである、請求項１～５のいずれか１項に記載の医薬組成物。 The pharmaceutical composition according to any one of claims 1 to 5, wherein the fucoidan is acetyl fucoidan.
  7. 海藻から分離したフコイダンともろみ酢とを混合した物質により腫瘍細胞の増殖率を抑制することを特徴とする腫瘍細胞の増殖率を抑制する方法。 A method for suppressing the growth rate of tumor cells, comprising suppressing the growth rate of tumor cells with a substance obtained by mixing fucoidan separated from seaweed and moromi vinegar.
  8. 海藻から分離したフコイダンともろみ酢とを混合した物質により腫瘍細胞の増殖率を抑制することを特徴とする腫瘍細胞の増殖率抑制物質。 A tumor cell growth rate inhibitor, which suppresses the growth rate of tumor cells by a substance mixed with fucoidan and moromi vinegar separated from seaweed.
  9. 前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク、ホンダワラ科などの海藻を由来としていることを特徴とする請求項７に記載の腫瘍細胞の増殖率を抑制する方法。 The blended amount of the moromi vinegar is 3% to 95%, and the fucoidan is derived from seaweeds such as mozuku, wakame, mekabu, kombu, hijiki, akamoku, hondawalidae, etc. To suppress the growth rate of tumor cells.
  10. 前記のもろみ酢の配合量を３％～95％とし、前記のフコイダンはモズク、ワカメ、メカブ、コンブ、ヒジキ、アカモク、ホンダワラ科などの海藻を由来としていることを特徴とする請求項８に記載の腫瘍細胞の増殖率抑制物質。 The blended amount of the moromi vinegar is 3% to 95%, and the fucoidan is derived from seaweed such as mozuku, seaweed, mekabu, kombu, hijiki, akamoku, hondawalidae, etc. A tumor cell growth rate inhibitor.
  11. 前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末及び／又はもろみ粕であることを特徴とする請求項７又は請求項９に記載の腫瘍細胞の増殖率を抑制する方法。 The moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi mash. A method for suppressing the growth rate of the described tumor cells.
  12. 前記のもろみ酢は、もろみ酢原液及び／又は除臭もろみ酢及び／又はもろみ酢粉末及び／又は除臭もろみ酢粉末及び／又はもろみ粕であることを特徴とする請求項８又は請求項１０に記載の腫瘍細胞の増殖率抑制物質。
                                                                                         The moromi vinegar is moromi vinegar stock solution and / or deodorized moromi vinegar and / or moromi vinegar powder and / or deodorized moromi vinegar powder and / or moromi mash. The tumor cell growth rate inhibitor as described.
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