JP2006199641A - Iron-adsorbing polymer substance, iron-containing polymer substance and method for producing the same - Google Patents
Iron-adsorbing polymer substance, iron-containing polymer substance and method for producing the same Download PDFInfo
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- JP2006199641A JP2006199641A JP2005014125A JP2005014125A JP2006199641A JP 2006199641 A JP2006199641 A JP 2006199641A JP 2005014125 A JP2005014125 A JP 2005014125A JP 2005014125 A JP2005014125 A JP 2005014125A JP 2006199641 A JP2006199641 A JP 2006199641A
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- iron
- polymer substance
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Abstract
Description
本発明は、鉄の吸収を促進し、鉄不足状態を改善する鉄吸収促進剤及び鉄分補強剤に関するものである。 The present invention relates to an iron absorption promoter and an iron reinforcing agent that promote iron absorption and improve iron deficiency.
鉄は、生命を維持する上で不可欠である必須微量栄養素の一つであって、酸素を運搬する赤血球中のヘモグロビンの主要成分であるとともに、筋肉中のミオグロビン及び体内の酸化還元に関与する酵素の成分として重要であり、生体内における増血作用に欠かせない因子である。
近年の国民栄養調査によれば、国の定めた標準値としての鉄分の摂取量は男女平均ではほぼ満たされているにも関わらず、有経女性の半数が鉄欠乏であるといわれており、また成長期の子供が鉄欠乏となる傾向が増加しているという指摘もあり、鉄欠乏によって生じる貧血等の諸症状の予防改善が必要とされている。また、献血や手術後、産後には血清鉄、ヘモグロビン含量等が減少するが、これが元の正常値に戻るまでに長期を必要としており、この回復期間をできる限り短縮することが望まれてもいる。
Iron is one of the essential micronutrients essential for maintaining life, and is a major component of hemoglobin in red blood cells that carry oxygen, as well as myoglobin in muscles and enzymes involved in redox in the body It is important as a component of blood and is an indispensable factor for blood-increasing action in vivo.
According to a recent National Nutrition Survey, even though the average intake of iron as a national standard is almost met on the average for men and women, half of the menstrual women are said to be iron deficient. In addition, it is pointed out that growing children have a tendency to become iron deficient, and it is necessary to prevent and improve various symptoms such as anemia caused by iron deficiency. In addition, serum iron and hemoglobin content decrease after blood donation, surgery, and postpartum, but it takes a long time to return to the original normal value, and it is desirable to shorten this recovery period as much as possible. Yes.
有経女性は成人男性の2倍近い鉄が必要と考えられているが、摂取鉄量は摂取カロリー量にほぼ比例していることから、男性に比較して摂取カロリーの少ない女性の摂取鉄量は必要量を下回ると考えられている。また、女性の嗜好性、ダイエット志向からも吸収率のよいヘム鉄を含む肉、レバーなどの摂取量が男性に比較して少ないことも問題であった。
鉄の欠乏は、出血、尿管内出血、妊娠、鉄欠乏食の摂取、腸からの鉄吸収異常等によって生じ、これが持続すると、鉄欠乏性貧血症に至る。従来、鉄の欠乏に際しては、クエン酸鉄、乳酸鉄、塩化第二鉄、硫酸鉄などの非ヘム鉄及び肉、レバー等に含まれるヘム鉄を摂取することやビタミンC、システインなど鉄の吸収を促進させる成分の多い食品を摂取することが勧められ、鉄の吸収を低下させるフィチン酸、リン酸、タンニン酸などを多く含む食品の摂取を避けることが望ましいとされている。
It is thought that women who need to have nearly twice as much iron as adult men need, but the amount of iron intake is almost proportional to the amount of calorie intake. Is considered to be below the required amount. Another problem is that the intake of meat and liver containing heme iron, which has a good absorption rate, is less than men's preference and diet-oriented.
Iron deficiency is caused by bleeding, intraurethral bleeding, pregnancy, intake of an iron deficient diet, abnormal absorption of iron from the intestine, etc., and if this persists, it leads to iron deficiency anemia. Conventionally, in the case of iron deficiency, ingestion of non-heme iron such as iron citrate, iron lactate, ferric chloride and iron sulfate and heme iron contained in meat, liver, etc., and absorption of iron such as vitamin C and cysteine It is recommended to eat foods with a lot of ingredients that promote the absorption of food, and it is desirable to avoid ingestion of foods rich in phytic acid, phosphoric acid, tannic acid, etc. that reduce iron absorption.
これまでに、鉄吸収促進活性を有するものとしては、食酢(例えば、特許文献1参照)、トリテルペン配糖体(例えば、特許文献2参照)、カルノシン、アンセリン、バレニン、及びπ−メチルヒスチジンの群から選ばれた1種以上のイミダゾール化合物(例えば、特許文献3参照)、グアーガム酵素分解物(例えば、特許文献4参照)、魚肉のタンパク分解酵素液から得られたペプチド(例えば、特許文献5参照)等が見出されているが、作用・効果が不十分な点や活性を保ったまま製剤に安定に配合することが困難であるという問題点が残されていた。 So far, those having iron absorption promoting activity include vinegar (see, for example, Patent Document 1), triterpene glycoside (see, for example, Patent Document 2), carnosine, anserine, valenin, and π-methylhistidine. One or more imidazole compounds selected from (for example, see Patent Document 3), guar gum enzyme degradation products (for example, see Patent Document 4), peptides obtained from fish proteolytic enzyme solution (for example, see Patent Document 5) However, there are still problems that are insufficient in action and effect and that it is difficult to stably blend into the preparation while maintaining the activity.
さらに世界に目を向けてみると、特に開発途上国において鉄欠乏貧血症は最も対策の遅れている健康問題の一つであり、WHOやユニセフなどの国際機関により経済的かつ効果的な鉄添加プログラムが実施されてきた(例えば、非特許文献1参照)。鉄を添加する食物は日常的に摂取する必要があり、小麦粉、米などの穀類や塩、砂糖、醤油などの調味料が鉄付加されてきた。アジア地域、特にベトナムや中国では、穀類より鉄吸収の効率が高い食品として鉄強化醤油を選択し、ヒト介入試験によりヘモグロビン値の上昇が確認されている(例えば、非特許文献2参照)。従って、これまでの研究では鉄を付加する媒体として醤油が有効であることは明らかにされているが、鉄吸収促進に関与する醤油成分については全く解明されていなかった。
鉄は、血中に吸収されにくい微量元素とされ、腸管から吸収される鉄は10%程度であることが知られている。それゆえ、鉄を大量に経口摂取しても、摂取した鉄の大部分はそのまま体外に排出されてしまうため、腸管からの鉄の吸収が促進される素材が望まれている。
本発明は、上記事情に鑑みなされたものであって、経済的、安全性に優れた鉄補強剤あるいは鉄吸収促進効果を有する物質及びその製造法を提供することを目的とする。
さらに本発明は、このような物質を添加した鉄吸収促進効果の生理活性を有する食品、飲料品、医薬品及び飼料を提供することを目的とする。
It is known that iron is a trace element that is difficult to be absorbed into the blood, and about 10% of iron is absorbed from the intestinal tract. Therefore, even if a large amount of iron is orally ingested, most of the ingested iron is discharged out of the body as it is, and therefore, a material that promotes the absorption of iron from the intestinal tract is desired.
This invention is made | formed in view of the said situation, Comprising: It aims at providing the substance which has the iron reinforcement agent excellent in economical and safety | security, or an iron absorption promotion effect, and its manufacturing method.
Furthermore, an object of the present invention is to provide foods, beverages, pharmaceuticals and feeds having physiological activity of promoting iron absorption to which such substances are added.
本発明者らは、鉄分補強効果や吸収促進効果を有する物質について検討を行った結果、醤油に含まれる高分子物質が高濃度に鉄を含有していること、この物質がさらに鉄イオンを吸着できること、また、鉄分補強剤として有効であることを発見し、本発明をなすに至った。さらに、醤油の主原料である大豆の発酵物にも同様の効果があることを見出し、本発明をなすに至った。
本発明の鉄吸着性を有する物質及び鉄含有高分子物質は、大豆を原料とし、麹菌などの微生物あるいは酵素を利用した発酵分解物から得ることができる。これら高分子物質は発酵分解物中に発現し、発酵分解物中の鉄イオンの存在量により、鉄吸着性高分子物質及び/又は鉄含有高分子物質として得られる。発酵分解物として醤油や醤油麹を代表例としてあげることができる。また、本発明の物質は、希アルコール可溶性、濃アルコール不溶性及び水可溶性であり、鉄吸着性高分子物質は分子量6,000以上、また、鉄含有高分子物質は鉄分200ppm程度以上を含有する。
As a result of studying a substance having an iron reinforcing effect and an absorption promoting effect, the present inventors have found that the polymer substance contained in soy sauce contains iron in a high concentration, and this substance further adsorbs iron ions. It has been discovered that it is possible and effective as an iron reinforcing agent, and the present invention has been made. Furthermore, it discovered that the fermented soybean of the main raw material of soy sauce had the same effect, and came to make this invention.
The iron-adsorbing substance and the iron-containing polymer substance of the present invention can be obtained from fermented decomposition products using soybeans as raw materials and microorganisms such as koji molds or enzymes. These polymer substances are expressed in the fermentation decomposition product, and are obtained as an iron-adsorbing polymer substance and / or an iron-containing polymer substance depending on the amount of iron ions in the fermentation decomposition product. Typical examples of the fermentation decomposition product include soy sauce and soy sauce cake. The substance of the present invention is dilute alcohol-soluble, concentrated alcohol-insoluble and water-soluble, the iron-adsorbing polymer substance has a molecular weight of 6,000 or more, and the iron-containing polymer substance contains about 200 ppm or more of iron.
すなわち本発明は、次の(1)〜(12)の鉄分補強剤及び鉄吸収促進剤に関する。
1.大豆を含む原料の発酵分解物から得られる、次の性質を有する鉄吸着性高分子物質。
(1)分画分子量6,000の透析膜で透析したとき、透析内液に残存する。
(2)水に可溶、アルコール等有機溶媒に不溶である。
(3)鉄をキレートする能力を有する。
2.大豆を含む原料の発酵分解物から得られる、次の性質を有する鉄含有高分子物質。
(1)分画分子量6,000の透析膜で透析したとき、透析内液に残存する。
(2)水に可溶、アルコール等有機溶媒に不溶である。
(3)鉄を200ppm以上含有する。
3.大豆を含む原料の発酵分解物、もしくは、その水抽出物、食塩水抽出物又は希アルコール抽出物を透析、限外ろ過及び/又はアルコール沈殿して得られる、請求項1又は2記載の鉄吸着性高分子物質又は鉄含有高分子物質。
4.請求項1又は3に記載の鉄吸着性高分子物質の溶液に鉄イオンを添加することにより得られる、鉄含有高分子物質。
5.大豆を含む発酵分解物が、醤油又は大豆を含む原料を用いた麹であることを特徴とする請求項 1から3のいずれかに記載の鉄吸着性高分子物質又は鉄含有高分子物質。
6.大豆を含む原料の発酵分解物、もしくはその水抽出物、食塩抽出物又は希アルコール抽出物を透析、限外ろ過及び/又はアルコール沈殿して高分子物質を採取することを特徴とする鉄吸着性高分子物質又は鉄含有高分子物質の製造法。
7.大豆を含む原料の発酵分解物、もしくはその水、食塩水あるいは希アルコール抽出物を得るにあたり、予め鉄イオンを添加しておくか、もしくは、得られた発酵分解物あるいはその抽出物に鉄イオンを添加し、その後、透析、限外ろ過及び/又はアルコール沈殿して高分子物質を採取することを特徴とする鉄含有高分子物質の製造法。
8.請求項2から5のいずれかに記載の鉄含有高分子物質を有効成分とし、他の鉄化合物を配合するか配合しない鉄分補強剤。
9.請求項1、3及び5のいずれかに記載の鉄吸着性高分子物質を有効成分とする鉄吸収促進剤。
10.請求項1から5のいずれかに記載の鉄吸着性高分子物質及び/又は鉄含有高分子物質を添加することを特徴とする食品。
11.請求項1から5のいずれかに記載の鉄吸吸着性高分子物質及び/又は鉄含有高分子物質を添加することを特徴とする飼料。
12.請求項1から5のいずれかに記載の鉄吸吸着性高分子物質及び/又は鉄含有高分子物質を添加することを特徴とする医薬品。
なお、本発明の医薬には、医薬部外品を含むものとする。
That is, this invention relates to the iron reinforcing agent and iron absorption promoter of following (1)-(12).
1. An iron-adsorbing polymer material obtained from fermentative decomposition products of raw materials containing soybeans and having the following properties.
(1) When dialyzed with a dialysis membrane having a molecular weight cut off of 6,000, it remains in the dialyzed solution.
(2) Soluble in water and insoluble in organic solvents such as alcohol.
(3) Ability to chelate iron.
2. An iron-containing polymer substance having the following properties obtained from a fermentative decomposition product of raw materials containing soybeans.
(1) When dialyzed with a dialysis membrane having a molecular weight cut off of 6,000, it remains in the dialyzed solution.
(2) Soluble in water and insoluble in organic solvents such as alcohol.
(3) Contains 200 ppm or more of iron.
3. The fermentative decomposition product of the raw material containing soybean, or its water extract, saline extract or dilute alcohol extract is obtained by dialysis, ultrafiltration and / or alcohol precipitation. Iron-adsorbing polymer material or iron-containing polymer material.
4. An iron-containing polymer material obtained by adding iron ions to a solution of the iron-adsorbing polymer material according to claim 1 or 3.
5. The fermentative decomposition product containing soybean is rice bran using a raw material containing soy sauce or soybean, Iron-adsorbing polymer material or iron-containing polymer material according to any one of claims 1 to 3 .
6. Iron characterized by collecting high-molecular substances by dialysis, ultrafiltration and / or alcohol precipitation of fermented decomposition products of raw materials containing soybeans, or water extracts, salt extracts or dilute alcohol extracts thereof. Method for producing adsorptive polymer substance or iron-containing polymer substance.
7. When obtaining fermented decomposition products of raw materials containing soybeans, or water, salt solution or dilute alcohol extracts thereof, iron ions are added in advance, or iron is added to the obtained fermentation decomposition products or extracts thereof. A method for producing an iron-containing polymer material, comprising adding ions and then collecting the polymer material by dialysis, ultrafiltration and / or alcohol precipitation.
8. An iron reinforcing agent comprising the iron-containing polymer substance according to any one of claims 2 to 5 as an active ingredient and containing or not containing other iron compounds.
9. An iron absorption promoter comprising as an active ingredient the iron-adsorptive polymer material according to any one of claims 1, 3 and 5.
10. A food comprising the iron-adsorbing polymer substance and / or the iron-containing polymer substance according to any one of claims 1 to 5.
11. A feed comprising the iron-absorbing polymer material and / or iron-containing polymer material according to any one of claims 1 to 5.
12. A pharmaceutical product comprising the iron-absorbing polymer substance and / or the iron-containing polymer substance according to any one of claims 1 to 5.
The medicament of the present invention includes quasi drugs.
本発明の大豆を原料とした発酵分解物から得られる高分子物質は、鉄吸着性作用及び/又は鉄を200ppm程度以上含有しており鉄吸収促進作用を有するので、鉄吸収、鉄強化のために飲食品あるいは医薬品として利用することができる。そして、安全性が高く、継続的な摂取も可能であり、かつ大量に供給することもでき、食品等への添加が容易であり、ヒト等の健康増進などに貢献するところが大である。さらに本発明の鉄吸着性高分子物質及び鉄含有高分子物質は、鉄の利用が不十分であるために起こる症状、例えば、貧血、頭痛、耳鳴り、息切れ、眩暈、運動障害、倦怠感等や献血後、手術後、産後の鉄欠乏状態への適用が期待される。
また、本発明の方法によると、このような効果のある高分子物質を容易に大量に製造することができる。
The polymer substance obtained from the fermented decomposition product of soybean of the present invention has an iron adsorptive action and / or an iron absorption promoting action containing about 200 ppm or more of iron. It can be used as food or drink or medicine. And it is highly safe, can be ingested continuously, can be supplied in large quantities, can be easily added to foods, etc., and contributes to health promotion of humans and the like. Furthermore, the iron-adsorptive polymer substance and iron-containing polymer substance of the present invention have symptoms caused by insufficient use of iron, such as anemia, headache, tinnitus, shortness of breath, dizziness, movement disorder, malaise, etc. Application to iron deficiency after blood donation, surgery, and postpartum is expected.
Further, according to the method of the present invention, a polymer substance having such an effect can be easily produced in large quantities.
大豆を蒸煮あるいは焙煎するなどの加熱処理を施し、これに、麹菌などの糸状菌を生育させることによって本発明に関わる活性成分を生成させる。糸状菌の生育を促進させるために、各種栄養源を補給することもできる。このようにして生成した本発明に関わる鉄吸着性の高分子物質は、水、食塩水あるいは30%(v/v)程度未満の希エタノール中で長期間発酵させても残存するものである。これらの一例として醤油の麹あるいは醤油を例示することができる。 A heat treatment such as steaming or roasting soybean is performed, and an active ingredient according to the present invention is generated by growing filamentous fungi such as koji molds. In order to promote the growth of filamentous fungi, various nutrient sources can also be supplemented. The iron-adsorptive polymer substance according to the present invention thus produced remains even if it is fermented for a long time in water, saline or dilute ethanol of less than about 30% (v / v). Examples of these are soy sauce cake or soy sauce.
本発明における鉄吸着性高分子物質又は鉄含有高分子物質は、発酵分解物中に発現し、これをそのまま利用することも可能である。さらに利用しやすくするために、以下に示すような手段で、抽出し、あるいはその高分子画分を濃縮することもできる。
発酵分解物が固体の場合、本発明の高分子物質を採取するためには、1から10重量部程度の水、食塩水、あるいは30%(v/v)程度未満の希エタノールを用いて本発明の生理活性成分を溶解することのできる条件で、1時間〜数日抽出し、そのろ液を使用する。
上記分解物の抽出ろ液を透析して透析内液を濃縮する方法、濃エタノールを添加して生成する不溶性物質をろ過あるいは遠心分離で集める方法、あるいは、これら液体を限外ろ過膜に通すことによって高分子物質を含有する画分である非透過液を集める方法、あるいはこの非透過液に濃エタノールを加えて不溶物を生成させ、それを回収する方法等が利用できる。
The iron-adsorbing polymer substance or iron-containing polymer substance in the present invention is expressed in a fermentation decomposition product and can be used as it is. In order to make it easier to use, it can be extracted or the polymer fraction can be concentrated by the following means.
When the fermented decomposition product is solid, in order to collect the polymer substance of the present invention, it is necessary to use about 1 to 10 parts by weight of water, saline, or diluted ethanol less than about 30% (v / v). Extraction is performed for 1 hour to several days under the condition that the physiologically active ingredient of the invention can be dissolved, and the filtrate is used.
Concentrating the dialyzed filtrate of the above decomposition product and concentrating the dialyzed solution, adding concentrated ethanol to collect the insoluble material produced by filtration or centrifugation, or passing these liquids through an ultrafiltration membrane A method of collecting a non-permeate that is a fraction containing a polymer substance by the above, or a method of adding concentrated ethanol to this non-permeate to produce an insoluble material and recovering it can be used.
本発明に関わる高分子物質を採取するために加えるエタノールの量は、高分子物質が不溶性となる濃度であればよく、最終エタノール濃度が30%(v/v)以上、望ましくは50%(v/v)以上になればよい。エタノールに代えてメタノールや2-プロパノール等のアルコールによっても本発明の高分子物質は回収できるが、安全性の面でエタノールが好ましい。本発明の高分子画分を採取した残りの液は、新たな原料から高分子物質を回収するために利用することも可能である。この液は添加したエタノールあるいはその他のアルコールとともにアミノ酸や低分子の糖質を含有するものであり、蒸留などの操作によってエタノールと分離する。エタノール等のアルコールは本発明において再利用でき、また、不揮発成分は調味料や食品として利用することもできる。 The amount of ethanol added to collect the polymer substance according to the present invention may be a concentration at which the polymer substance becomes insoluble, and the final ethanol concentration is 30% (v / v) or more, preferably 50% (v / v) or more. Although the polymer substance of the present invention can be recovered by using alcohol such as methanol or 2-propanol instead of ethanol, ethanol is preferred from the viewpoint of safety. The remaining liquid obtained by collecting the polymer fraction of the present invention can be used for recovering the polymer material from a new raw material. This solution contains amino acids and low molecular weight carbohydrates together with added ethanol or other alcohols, and is separated from ethanol by an operation such as distillation. Alcohols such as ethanol can be reused in the present invention, and non-volatile components can be used as seasonings and foods.
また、本発明の高分子物質は醤油を原料として製造した場合、高分子物質中には約0.1%の鉄が含有された鉄含有高分子物質であり、鉄分補強剤としての利用が可能である。また、麹の水抽出物から得られる高分子物質中の鉄含量は、醤油から得られるものより低いが、200ppm程度以上の鉄を含有した鉄含有高分子物質は、特に鉄を追加しなくとも鉄補強剤として利用することができる。
さらに、本発明に関わる鉄含有高分子物質は、硫酸第一鉄などの鉄イオンを含む溶液に上記鉄吸着性高分子物質を添加して溶解することにより製造することができる。また、醤油、あるいは麹を水、食塩水、希エタノールで抽出した抽出液に硫酸第一鉄などの鉄イオンを添加することによって製造することもできる。これらの溶液を透析して透析内液を採取する、限外ろ過により非透過液を採取する、あるいはエタノールを加えて沈殿させる等、あるいはこれらを適宜組み合わせる等の方法によって、鉄分が強化された本発明に関わる高分子物質が得られる。
得られた高分子物質は、水などに溶解した形態、粉末化した形態、あるいはそのまま利用することが可能であり、製剤としてもよく、また飲食品、飼料、医薬品(医薬部外品も含む)などに適宜配合することができる。
In addition, when the polymer material of the present invention is produced using soy sauce as a raw material, the polymer material is an iron-containing polymer material containing about 0.1% iron, and can be used as an iron reinforcing agent. . Further, the iron content in the polymer material obtained from the water extract of persimmon is lower than that obtained from soy sauce, but the iron-containing polymer material containing about 200 ppm or more of iron does not need to be added with iron. It can be used as an iron reinforcing agent.
Furthermore, the iron-containing polymer substance according to the present invention can be produced by adding and dissolving the iron-adsorptive polymer substance in a solution containing iron ions such as ferrous sulfate. Moreover, it can also manufacture by adding iron ions, such as ferrous sulfate, to the extract which extracted soy sauce or rice cake with water, salt solution, and diluted ethanol. The iron content is enhanced by methods such as dialysis of these solutions to collect dialysis internal fluid, collection of non-permeate by ultrafiltration, precipitation by adding ethanol, or a combination thereof. A polymer substance related to the invention is obtained.
The obtained high molecular weight substance can be used in the form dissolved in water, powdered form, or as it is, and may be used as a preparation, and it may be a food, drink, feed, pharmaceutical (including quasi drugs). It can mix | blend suitably.
本発明の鉄吸着性高分子物質及び鉄含有高分子物質は、上記の方法により得られた抽出物をそのまま直接使用してもよく、スプレードライや凍結乾燥などの常法によって乾燥して用いることもできる。
一般的には適当な液体担体に溶解するかもしくは分散させ、又は、適当な粉末担体と混合するかもしくはこれに吸着させ、場合によっては、さらにこれらに乳化剤、分散剤、懸濁剤、展着剤、浸透剤、湿潤剤、安定剤等を添加し、乳剤、油剤、水和剤、散剤、錠剤、カプセル剤、液剤等の製剤として使用する。使用量は鉄分補強剤として用いるときは、1日あたり食品の場合5〜10mg程度、また、医薬品の場合10〜100mgの鉄が摂取できるようにすることが好ましい。
For the iron-adsorbing polymer substance and iron-containing polymer substance of the present invention, the extract obtained by the above method may be used directly as it is, or it may be used after being dried by a conventional method such as spray drying or freeze drying. You can also.
It is generally dissolved or dispersed in a suitable liquid carrier, or mixed with or adsorbed to a suitable powder carrier, and in some cases, further emulsifier, dispersant, suspending agent, spreading Additives, penetrants, wetting agents, stabilizers, etc. are added and used as preparations such as emulsions, oils, wettable powders, powders, tablets, capsules, and liquids. When used as an iron reinforcing agent, the amount used is preferably about 5 to 10 mg per day for foods and about 10 to 100 mg for pharmaceuticals.
鉄強化飲食物を得るに当たって、その本発明の高分子物質を飲食物に添加する方法としては、通常一般的に行われている方法でよい。
これらの飲食物としては、チューインガム,キャンディ,錠菓,グミ、ゼリー,チョコレート,ビスケット又はスナック等の菓子、アイスクリーム,シャーベット又は氷菓等の冷菓、飲料、プリン、ジャム、乳製品等が挙げられ、これらの飲食物を日常的に摂取することにより鉄吸収を強化することが可能となる。
In obtaining an iron-reinforced food or drink, the method of adding the polymer substance of the present invention to the food or drink may be a generally performed method.
Examples of these foods and beverages include chewing gum, candy, tablet confectionery, gummi, jelly, chocolate, biscuits or snacks and other confectionery, ice cream, sorbet or ice confectionary frozen confectionery, beverages, pudding, jam, dairy products, etc. It is possible to enhance iron absorption by daily intake of these foods and drinks.
本発明の高分子物質は、医薬品として鉄分補給の必要な女性や幼児に鉄分を高めるためにも用いることができる。剤形は得に限定されるものではなく、製剤学的に許容することのできる担体との併用も可能である。投与形態としては、特に限定がなく、例えば、散剤、細粒剤、顆粒剤、錠剤、カプセル剤、懸濁液、エマルジョン剤、シロップ剤、エキス剤、もしくは丸剤などの経口剤を挙げることができる。経口剤は、賦形剤、結合剤、崩壊剤、界面活性剤、潤沢剤、流動性促進剤、希釈剤、保存剤、着色剤、香料、安定化剤、保湿剤、防腐剤、又は酸化防止剤等を用いて、常法に従って製造することができる。 The polymer substance of the present invention can also be used to increase iron content in women and infants who need iron supplementation as pharmaceuticals. The dosage form is not particularly limited, and can be used in combination with a pharmaceutically acceptable carrier. The dosage form is not particularly limited, and examples thereof include oral preparations such as powders, fine granules, granules, tablets, capsules, suspensions, emulsions, syrups, extracts, or pills. it can. Oral agents are excipients, binders, disintegrants, surfactants, lubricants, fluidity promoters, diluents, preservatives, colorants, fragrances, stabilizers, humectants, preservatives, or antioxidants It can manufacture according to a conventional method using an agent.
さらに本発明の高分子物質を鉄吸収強化の目的で使用する場合、適宜、ビタミンCその他の鉄吸収代謝促進剤、鉄化合物などを混合することはさらに効果を高める上で有効である。また、本願発明の効果を妨げない範囲で、例えば、栄養剤、微量元素などの各種物質を混合することもできる。鉄化合物としては、特に限定されることなく、塩化鉄 、硫酸第一鉄 、クエン酸第一鉄 、クエン酸鉄 アンモニウム、クエン酸鉄ナトリウム、乳酸鉄 、ピロリン酸鉄 その他無機ないし有機の鉄化合物が適宜使用できるし、配合量も市販鉄剤と同様にすればよい。本発明においては、高い鉄の吸収効果が期待できるので、少量の鉄分を配合してもこれを有効に利用することができる。 Furthermore, when the polymer substance of the present invention is used for the purpose of enhancing iron absorption, it is effective to appropriately mix vitamin C and other iron absorption metabolism promoters, iron compounds and the like. Moreover, various substances, such as a nutrient and a trace element, can also be mixed in the range which does not prevent the effect of this invention. Examples of the iron compound include, but are not limited to, iron chloride, ferrous sulfate, ferrous citrate, ammonium iron citrate, sodium iron citrate, iron lactate, iron pyrophosphate, and other inorganic or organic iron compounds. It can be used appropriately, and the blending amount may be the same as that of the commercially available iron agent. In the present invention, since a high iron absorption effect can be expected, even if a small amount of iron is blended, it can be used effectively.
本発明の高分子物質を得る手段の一例を以下に示す。しかし、本発明はこのような方法に特に限定されるものではない。 An example of means for obtaining the polymer substance of the present invention is shown below. However, the present invention is not particularly limited to such a method.
醤油から得られた高分子物質の鉄補強及び吸収促進作用
(醤油から得られた高分子物質)
脱脂加工大豆、丸大豆及び小麦を主原料とした醤油10 Lを、食塩濃度約3%まで脱塩した後エタノール20Lを加えて混合し、遠心分離によって沈殿物を採取し、これを凍結乾燥し約100gの乾燥物を得て、これを粉砕して高分子物質とした。この乾燥高分子物質には鉄が1000ppm含有されており、さらに鉄キレート能を有していた。この鉄含量は、原料として用いた醤油に含まれる大部分の鉄が高分子成分に吸着されていることを示唆する。
この高分子物質は、分画分子量6,000の透析膜で透析したとき、透析内液に残存し、水、食塩水、希アルコールに可溶、濃アルコール、エチルエーテル等の有機溶媒に不溶である。
この、高分子物質を用いてヒト摂取評価試験を行った。すなわち、試験食品は1カプセルあたり高分子物質150mg(鉄分として0.15mg)と、結晶セルロース、微量のショ糖脂肪酸エステル及び二酸化珪素を混合した粉末をカプセルに充填したものである。また、対照食品は高分子物質を添加せずに上記と同配合で調製した粉末をカプセルに充填したものである。
(被験者)
被験者は有経女性45名で、本試験の目的、方法などを十分に説明し、ヘルシンキ宣言の主旨に従い本人の文書による同意を得て評価試験を実施した。
Iron reinforcement and absorption promotion action of polymer material obtained from soy sauce (polymer material obtained from soy sauce)
10 L of soy sauce made mainly from defatted soybeans, whole soybeans and wheat is desalted to a salt concentration of about 3%, mixed with 20 L of ethanol, and the precipitate is collected by centrifugation and freeze-dried. About 100 g of a dried product was obtained and pulverized to obtain a polymer material. This dry polymer material contained 1000 ppm of iron and had iron chelating ability. This iron content suggests that most of the iron contained in the soy sauce used as a raw material is adsorbed by the polymer component.
This high molecular weight substance remains in the dialysis internal solution when dialyzed with a dialysis membrane having a molecular weight cut off of 6,000, is soluble in water, saline and dilute alcohol, and is insoluble in organic solvents such as concentrated alcohol and ethyl ether.
A human intake evaluation test was conducted using this polymer substance. That is, the test food is one in which capsules are filled with a powder containing 150 mg of a high-molecular substance (0.15 mg as iron) per capsule, crystalline cellulose, a small amount of sucrose fatty acid ester and silicon dioxide. In addition, the control food is a capsule filled with a powder prepared with the same composition as above without adding a polymer substance.
(subject)
The subjects were 45 meridian women, who fully explained the purpose and method of this study, and conducted an evaluation study with their written consent in accordance with the purpose of the Declaration of Helsinki.
(ヒト摂取評価試験)
表1のように、被験者を高分子物質摂取群(試験食品、鉄含有量0.15mg/1カプセル)とプラセボ摂取群(対照食品、鉄含有量0.0mg/1カプセル)の二群に割り付けた。被験者の所属する群が誰にもわからない状態でその効果を調べる二重盲検比較試験を行った。試験食品群(22名)は、高分子物質を含む試験食品を朝夕2回に分けて2カプセルずつ、1日あたり合計4カプセル(鉄分として0.6mg)を摂取するように指導した。一方、対照食品群(23名)は、高分子物質を含まない対照食品を朝夕2回に分けて2カプセルずつ、1日あたり合計4カプセルを摂取するように指導した。また、日常の食生活や活動に一切の制限を設けてはいない。摂取前、摂取4週後に採血を行い、赤血球数、血清鉄、ヘマトクリット、血色素量を検査した。血液検査結果を表2に示す。二群間の比較は、student-t検定を行い、危険率5%未満を有意差ありと判定し、表中の*は危険率5%未満、**は危険率1%未満であること及びNSは有意差なしであることを示す。表からわかるように、血清鉄、ヘマトクリット、血色素量が対照区に較べて統計的有意に改善され、また赤血球数は危険率10%未満であり改善傾向であることが明確である。
一般成人の1日当たりの鉄平均摂取量は、厚生労働省『国民栄養の現状』2002年版によるとで約11mgであり、また、保健機能食品(栄養機能食品)においては1日に5〜10mg摂取できる食品にするよう定められている。本試験における試験食品から来る摂取量は僅か0.6mgであるが、表2に示したように対照食品に比して、試験食品では鉄吸収が効率的に行われていることが明確に示されている。この結果から、本発明に関わる鉄含有高分子は鉄補強剤として有用であるとともに、試験食品から供給される鉄以外の、通常食品に存在する鉄の吸収を促進している可能性が示唆された。
(Human intake evaluation test)
As shown in Table 1, subjects were assigned to two groups: a polymer substance intake group (test food, iron content 0.15 mg / 1 capsule) and a placebo intake group (control food, iron content 0.0 mg / 1 capsule). A double-blind comparative study was conducted to examine the effect of the test subject in a state where no one knew the group to which the subject belonged. The test food group (22 persons) was instructed to take the test food containing the polymer substance twice a day in the morning and evening to take 2 capsules a total of 4 capsules per day (0.6 mg of iron). On the other hand, the control food group (23 persons) was instructed to take a total of 4 capsules per day, divided into 2 mornings and evenings for the control foods that do not contain a polymer substance. In addition, there are no restrictions on daily eating habits and activities. Blood samples were collected before ingestion and 4 weeks after ingestion, and the red blood cell count, serum iron, hematocrit, and hemoglobin content were examined. The blood test results are shown in Table 2. For comparison between the two groups, a student-t test was performed, and a risk rate of less than 5% was determined to be significant, * in the table was less than 5% risk rate, ** was less than 1% risk rate, and NS indicates no significant difference. As can be seen from the table, serum iron, hematocrit, and hemoglobin content are statistically significantly improved compared to the control group, and the red blood cell count is less than 10%, which is clearly improving.
According to the Ministry of Health, Labor and Welfare's “National Nutrition Status” 2002 edition, the average daily iron intake for general adults is approximately 11 mg. It is stipulated to be food. The intake from the test food in this study is only 0.6 mg, but it is clearly shown that the test food is more efficiently absorbing iron than the control food, as shown in Table 2. ing. This result suggests that the iron-containing polymer according to the present invention is useful as an iron reinforcing agent and promotes absorption of iron present in normal foods other than iron supplied from test foods. It was.
実施例1の醤油から得られた高分子物質の粉末1gを水100mlに溶解し、20mgの硫酸第一鉄を少量の水に溶解して添加し、撹拌後、分画分子量6,000の透析チューブに詰めて流水中で1夜透析して、未吸着の硫酸第一鉄を除去した。その後、透析内液を凍結乾燥して得られた粉末は、鉄を1300ppm含有しており、醤油から得られた鉄含有高分子物質がさらに鉄吸着性を持つことが明らかであった。 Dissolve 1 g of the polymer substance powder obtained from the soy sauce of Example 1 in 100 ml of water, add 20 mg of ferrous sulfate dissolved in a small amount of water, and after stirring, add it to a dialysis tube with a molecular weight cut off of 6,000. Packed and dialyzed overnight in running water to remove unadsorbed ferrous sulfate. Thereafter, the powder obtained by freeze-drying the dialysis internal solution contained 1300 ppm of iron, and it was clear that the iron-containing polymer substance obtained from soy sauce further had iron adsorption properties.
麹からの製造方法
(高分子物質の製造)
3L容三角フラスコに大豆100gをいれ、熱水120mlを加えた後30分間放置した。続いて、焙煎割砕小麦90gを加えよく撹拌後、121℃で45分間オートクレーブ処理を行った。放冷後、醤油麹菌の胞子(Aspergillus oryzae)1gを植菌しよく撹拌した。その後、30℃に保持したウォーターバスで48時間静置培養を行った。その間、撹拌のため2回手入れ(20時間後及び30時間後)を行った。
培養した麹の一部(90g)に純水150mlを加え、10,000rpmで15分間ホモジネートを行った。ホモジネート液を7,000rpmで30分間遠心分離を行い、上清を回収して各麹の水抽出液とした。
水抽出物は分画分子量6,000の透析チューブに詰めて流水中で1夜透析後、透析内液にエタノールを60%になるように添加して得られた沈殿物を遠心分離して採取した。この沈殿物を、50℃減圧下で乾燥して本発明の鉄吸着性を有する鉄含有高分子物質を得た。この乾燥物は鉄キレート力があり、また鉄が500ppm含有されていた。
さらに、硫酸第一鉄2mgを溶解した水20mlに上記高分子物質0.1gを添加して撹拌溶解後、分画分子量6,000の透析チューブに詰めて1夜流水中で透析し未吸着の硫酸第一鉄を除去後、透析内液を凍結乾燥した。この乾燥物には、1500ppmの鉄が含有されていた。
2つの乾燥物は、水、食塩水、希アルコールに可溶、濃アルコール、エチルエーテル等の有機溶媒に不溶であった。
Manufacturing method from straw (Manufacturing polymer material)
100 g of soybeans was placed in a 3 L Erlenmeyer flask, 120 ml of hot water was added, and the mixture was left for 30 minutes. Subsequently, 90 g of roasted cracked wheat was added and stirred well, followed by autoclaving at 121 ° C. for 45 minutes. After standing to cool, 1 g of Aspergillus oryzae spores were inoculated and stirred well. Thereafter, static culture was performed in a water bath maintained at 30 ° C. for 48 hours. In the meantime, maintenance was carried out twice for stirring (after 20 hours and after 30 hours).
150 ml of pure water was added to a part (90 g) of the cultured koji and homogenized at 10,000 rpm for 15 minutes. The homogenate solution was centrifuged at 7,000 rpm for 30 minutes, and the supernatant was collected to obtain a water extract of each bottle.
The water extract was packed in a dialysis tube having a molecular weight cut off of 6,000, dialyzed overnight in running water, and the precipitate obtained by adding ethanol to the dialyzed solution to 60% was collected by centrifugation. This precipitate was dried under reduced pressure at 50 ° C. to obtain an iron-containing polymer substance having iron adsorptivity according to the present invention. This dried product had an iron chelating power and contained 500 ppm of iron.
Furthermore, after adding 0.1 g of the above-mentioned polymer substance to 20 ml of water in which 2 mg of ferrous sulfate is dissolved, stirring and dissolving, the mixture is packed in a dialysis tube with a molecular weight cut off of 6,000 and dialyzed in running water overnight. After removing iron, the dialyzed solution was lyophilized. This dried product contained 1500 ppm of iron.
The two dried products were soluble in water, saline and dilute alcohol, and insoluble in organic solvents such as concentrated alcohol and ethyl ether.
(酵素による製造方法)
3L容三角フラスコにフスマ50gをいれ、水120mlを加えた後よく撹拌混合し、その後オートクレーブにて121℃30分殺菌した。冷却後、Asp.orizaeの胞子0.05gを添加しよく撹拌後、30℃の水浴中で96時間培養した。培養中、20時間、40時間後に撹拌した。この培養物に水300mlを加えホモジナイズした後、遠心分離して200mlの抽出物を得た。この抽出物を0.45μmのフィルターでろ過し、無菌の酵素液とした。
一方、200mlの三角フラスコに大豆20gをいれ、熱水30mlを加え撹拌後30分放置し、その後121℃でオートクレーブして殺菌、冷却した。これに無菌的に上記フスマ麹から得た無菌の酵素液100mlを加え、30℃の水浴中で96時間振とうした後、遠心分離して80mlの発酵分解液を得た。この発酵分解液30mlを分画分子量6,000の透析チューブに詰めて1夜流水中で透析して透析内液を凍結乾燥して乾燥物を得た。この乾燥物は鉄キレート力を示し、200ppmの鉄を含有していた。2つの乾燥物は水に可溶、濃アルコール、エチルエーテル等の有機溶媒に不溶であった。
また、残りの発酵分解液50mlに少量の水に溶解した5mgの硫酸第一鉄を添加して撹拌後、流水中で1晩透析し、透析内液を凍結乾燥したところ、1200ppmの鉄を含有した高分子粉末が得られた。
(Production method using enzymes)
50 g of bran was placed in a 3 L Erlenmeyer flask, 120 ml of water was added, and the mixture was well stirred and mixed, and then sterilized at 121 ° C. for 30 minutes in an autoclave. After cooling, 0.05 g of Asp. Orizae spores were added and stirred well, followed by culturing in a 30 ° C. water bath for 96 hours. During the cultivation, the mixture was stirred after 20 hours and 40 hours. The culture was homogenized with 300 ml of water, and then centrifuged to obtain 200 ml of extract. This extract was filtered through a 0.45 μm filter to obtain a sterile enzyme solution.
On the other hand, 20 g of soybeans was put into a 200 ml Erlenmeyer flask, 30 ml of hot water was added, and the mixture was stirred and allowed to stand for 30 minutes. To this, 100 ml of an aseptic enzyme solution obtained from the above bran koji was aseptically added, shaken in a 30 ° C. water bath for 96 hours, and then centrifuged to obtain 80 ml of a fermentation decomposition solution. 30 ml of this fermentation decomposition solution was packed in a dialysis tube having a molecular weight cut off of 6,000, dialyzed in running water overnight, and the dialysis internal solution was lyophilized to obtain a dried product. This dried product exhibited iron chelating power and contained 200 ppm of iron. The two dried products were soluble in water and insoluble in organic solvents such as concentrated alcohol and ethyl ether.
In addition, 5 mg of ferrous sulfate dissolved in a small amount of water was added to 50 ml of the remaining fermentation decomposition solution, stirred, dialyzed overnight in running water, and the dialysis internal solution was freeze-dried. It contained 1200 ppm of iron. A polymer powder was obtained.
大豆麹10kgに鉄イオンとして10mg/L の硫酸第一鉄を含む15%のエタノールを30L添加して1週間冷蔵保管し、その後ろ過して抽出液20Lを得た。これを、分画分子量6,000の限外ろ過膜を付した限外ろ過機にかけ、非透過液2Lを得た。これに4Lのエタノールを加えて撹拌後1日静置した。生成した沈殿物をデカンテーションによって集め、これを50℃で減圧して乾燥粉末300gを得た。この粉末は、鉄1100ppmを含有しており、水に溶解して透析しても減少することがなく、鉄は高分子物質に取り込まれていると推測できた。この粉末は、水、食塩水、希アルコールに可溶、濃アルコール、エチルエーテル等の有機溶媒に不溶であった。 30 L of 15% ethanol containing 10 mg / L ferrous sulfate as iron ions was added to 10 kg of soybean meal and refrigerated for 1 week, followed by filtration to obtain 20 L of extract. This was applied to an ultrafilter equipped with an ultrafiltration membrane having a molecular weight cut off of 6,000 to obtain 2 L of a non-permeate. 4 L of ethanol was added thereto, and the mixture was stirred and allowed to stand for 1 day. The produced precipitate was collected by decantation, and this was decompressed at 50 ° C. to obtain 300 g of a dry powder. This powder contained 1100 ppm of iron and did not decrease even when dissolved in water and dialyzed, and it was assumed that iron was taken up by the polymer substance. This powder was soluble in water, saline, dilute alcohol, and insoluble in organic solvents such as concentrated alcohol and ethyl ether.
(鉄強化醤油)
実施例1と同様にして得られた鉄吸着性高分子物質50gとクエン酸鉄2.4gを市販醤油1,000mlに添加し、混合溶解して鉄強化醤油を作成した。この醤油は10ml中に鉄約5mgを含有する。
また、通常醤油にクエン酸第鉄を添加して保存すると褐変速度が非常に大きくなり保存性が劣るが、本発明の鉄吸着性高分子物質を添加した醤油の褐変速度はクエン酸第鉄のみを添加した醤油に較べて明らかに小さく、褐変抑制効果が示唆された。
(Iron-enriched soy sauce)
50 g of the iron-adsorbing polymer material obtained in the same manner as in Example 1 and 2.4 g of iron citrate were added to 1,000 ml of commercially available soy sauce, mixed and dissolved to prepare iron-reinforced soy sauce. This soy sauce contains about 5 mg of iron in 10 ml.
In addition, when ferrous citrate is added to normal soy sauce and stored, the browning rate becomes very large and storage stability is poor, but the browning rate of soy sauce to which the iron-adsorbing polymer material of the present invention is added is only ferrous citrate. This was clearly smaller than the soy sauce added with sucrose, suggesting an effect of inhibiting browning.
(粉末食品の処方)
実施例2と同様にして得られた凍結乾燥粉末10%、馬鈴薯澱粉20%、乳糖70%を混合して粉末食品を得た。
この粉末10gには鉄が約1mg含まれている。
(Prescription of powdered food)
A powdered food was obtained by mixing 10% of freeze-dried powder, 20% of potato starch and 70% of lactose obtained in the same manner as in Example 2.
10 g of this powder contains about 1 mg of iron.
(飲料の処方)
実施例2と同様にして得られた凍結乾燥粉末2.5%、オレンジ果汁5%、異性化糖15%、アスコルビン酸0.1%、香料0.1%及び水74.8%を混合してオレンジ果汁飲料を得た。この飲料200mlには鉄が約5mg含有されている。
(Beverage prescription)
An orange juice drink was obtained by mixing 2.5% of the freeze-dried powder obtained in the same manner as in Example 2, 5% orange juice, 15% isomerized sugar, 0.1% ascorbic acid, 0.1% fragrance and 74.8% water. 200ml of this beverage contains about 5mg of iron.
(医薬品)
実施例2と同様にして得られた乾燥粉末50%、デキストリン35%+フマル酸鉄15%を混合し、0.2gをゼラチンカプセルに充填する。この1カプセルには約10mgの鉄を含有する。
(Medicine)
50% of the dry powder obtained in the same manner as in Example 2, 35% dextrin and 15% iron fumarate are mixed, and 0.2 g is filled into a gelatin capsule. Each capsule contains about 10 mg of iron.
本発明によって得られる高分子物質は鉄吸収促進作用を有し、鉄吸収促進剤、鉄吸収促進飲食品、飼料等として利用することができ、鉄の利用が不十分であるために起こる症状、例えば、貧血、頭痛、耳鳴り、息切れ、眩暈、運動障害、倦怠感等や献血後、手術後、産後の鉄欠乏状態への適用が期待される。 The polymer substance obtained by the present invention has an iron absorption promoting action, and can be used as an iron absorption promoter, iron absorption promoting food and drink, feed, etc., symptoms caused by insufficient use of iron, For example, it is expected to be applied to iron deficiency after anemia, headache, tinnitus, shortness of breath, dizziness, movement disorder, malaise, blood donation, surgery, and postpartum.
Claims (12)
(1)分画分子量6,000の透析膜で透析したとき、透析内液に残存する。
(2)水に可溶、アルコール等有機溶媒に不溶である。
(3)鉄をキレートする能力を有する。 An iron-adsorbing polymer material obtained from a fermentative decomposition product of raw materials containing soybeans and having the following properties.
(1) When dialyzed with a dialysis membrane having a molecular weight cut off of 6,000, it remains in the dialyzed solution.
(2) Soluble in water and insoluble in organic solvents such as alcohol.
(3) It has the ability to chelate iron.
(1)分画分子量6,000の透析膜で透析したとき、透析内液に残存する。
(2)水に可溶、アルコール等有機溶媒に不溶である。
(3)鉄を200ppm以上含有する。 An iron-containing polymer substance having the following properties obtained from a fermentative decomposition product of raw materials containing soybeans.
(1) When dialyzed with a dialysis membrane having a molecular weight cut off of 6,000, it remains in the dialyzed solution.
(2) Soluble in water and insoluble in organic solvents such as alcohol.
(3) Containing 200 ppm or more of iron.
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Cited By (4)
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JP2008088151A (en) * | 2006-09-08 | 2008-04-17 | Higashimaru Shoyu Co Ltd | Application of polymer material included in soy sauce |
JP2012162485A (en) * | 2011-02-07 | 2012-08-30 | Higashimaru Shoyu Co Ltd | Iron absorption promoter |
CN103493973A (en) * | 2013-09-30 | 2014-01-08 | 河南亚卫动物药业有限公司 | Compound fermentation hog powder for livestock and poultry and preparation method |
WO2014040122A1 (en) * | 2012-09-11 | 2014-03-20 | Dakota Star Capital Llc | Nutritional supplement containing iron |
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Cited By (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP2008088151A (en) * | 2006-09-08 | 2008-04-17 | Higashimaru Shoyu Co Ltd | Application of polymer material included in soy sauce |
JP2012162485A (en) * | 2011-02-07 | 2012-08-30 | Higashimaru Shoyu Co Ltd | Iron absorption promoter |
WO2014040122A1 (en) * | 2012-09-11 | 2014-03-20 | Dakota Star Capital Llc | Nutritional supplement containing iron |
CN104717968A (en) * | 2012-09-11 | 2015-06-17 | 达科他星都有限公司 | Nutritional supplement containing iron |
JP2015532827A (en) * | 2012-09-11 | 2015-11-16 | ダコタ スター キャピタル エルエルシー | Nutritional supplements containing iron |
US11478519B2 (en) | 2012-09-11 | 2022-10-25 | Cura Global Health (Bvi) Limited | Nutritional supplement containing iron |
CN103493973A (en) * | 2013-09-30 | 2014-01-08 | 河南亚卫动物药业有限公司 | Compound fermentation hog powder for livestock and poultry and preparation method |
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