WO2023190666A1 - ケイ素化合物水溶液の製造方法 - Google Patents

ケイ素化合物水溶液の製造方法 Download PDF

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WO2023190666A1
WO2023190666A1 PCT/JP2023/012766 JP2023012766W WO2023190666A1 WO 2023190666 A1 WO2023190666 A1 WO 2023190666A1 JP 2023012766 W JP2023012766 W JP 2023012766W WO 2023190666 A1 WO2023190666 A1 WO 2023190666A1
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silicon compound
silicon
water
producing
rice husk
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French (fr)
Japanese (ja)
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晃 前ノ園
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K Wort Science Co Ltd
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K Wort Science Co Ltd
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    • AHUMAN NECESSITIES
    • A23FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23LFOODS, FOODSTUFFS OR NON-ALCOHOLIC BEVERAGES, NOT OTHERWISE PROVIDED FOR; PREPARATION OR TREATMENT THEREOF
    • A23L29/00Foods or foodstuffs containing additives; Preparation or treatment thereof
    • AHUMAN NECESSITIES
    • A23FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23LFOODS, FOODSTUFFS OR NON-ALCOHOLIC BEVERAGES, NOT OTHERWISE PROVIDED FOR; PREPARATION OR TREATMENT THEREOF
    • A23L33/00Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof
    • A23L33/10Modifying nutritive qualities of foods; Dietetic products; Preparation or treatment thereof using additives
    • A23L33/105Plant extracts, their artificial duplicates or their derivatives
    • AHUMAN NECESSITIES
    • A23FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23LFOODS, FOODSTUFFS OR NON-ALCOHOLIC BEVERAGES, NOT OTHERWISE PROVIDED FOR; PREPARATION OR TREATMENT THEREOF
    • A23L5/00Preparation or treatment of foods or foodstuffs, in general; Food or foodstuffs obtained thereby; Materials therefor
    • AHUMAN NECESSITIES
    • A23FOODS OR FOODSTUFFS; TREATMENT THEREOF, NOT COVERED BY OTHER CLASSES
    • A23LFOODS, FOODSTUFFS OR NON-ALCOHOLIC BEVERAGES, NOT OTHERWISE PROVIDED FOR; PREPARATION OR TREATMENT THEREOF
    • A23L7/00Cereal-derived products; Malt products; Preparation or treatment thereof
    • A23L7/10Cereal-derived products
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K33/00Medicinal preparations containing inorganic active ingredients
    • AHUMAN NECESSITIES
    • A61MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61KPREPARATIONS FOR MEDICAL, DENTAL OR TOILETRY PURPOSES
    • A61K8/00Cosmetics or similar toiletry preparations
    • A61K8/18Cosmetics or similar toiletry preparations characterised by the composition
    • A61K8/19Cosmetics or similar toiletry preparations characterised by the composition containing inorganic ingredients
    • A61K8/25Silicon; Compounds thereof
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00Silicon; Compounds thereof
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B33/00Silicon; Compounds thereof
    • C01B33/113Silicon oxides; Hydrates thereof

Definitions

  • the present invention relates to a method for producing an aqueous silicon compound solution using rice husk as a raw material, and furthermore, a silicon compound-containing food or drink using the method for producing an aqueous silicon compound solution; an agent for preventing and improving disorders of muscles, blood vessels, or bones;
  • This invention relates to a method for producing silicon-containing materials.
  • the present invention also relates to silicon compound aqueous solutions, silicon-containing materials, etc. produced by the above production method.
  • Patent Document 1 describes a method for producing a fire-resistant heat insulating material, in which calcium silicate hydrate crystals obtained by suspending rice husk ash and lime raw materials in water and reacting them are molded and dried.
  • white amorphous rice husk ash is obtained by heating rice husks in an oxidizing atmosphere to, for example, 600°C to burn and ash, which is used as a raw material (Patent Document 1 Claim 1, Example 1, etc.).
  • Patent Document 2 describes a method for producing amorphous silica in which rice husks are immersed in an aqueous solution containing an oxidizing substance, and then heated and oxidized in the presence of oxygen.
  • rice husk is oxidized by heating in the presence of air to sufficiently reduce the organic material in the rice husk, and this is used as a raw material (Claim 9 of Patent Document 2, [0010] , [0016], [0020], etc.).
  • Patent Document 3 describes a mushroom mycelium growth promoter and fruiting body formation promoter whose active ingredient is an extract obtained by extracting rice husk with an aqueous solvent such as alcohol.
  • Patent Document 3 uses organic substances in rice husks to promote growth, etc., and does not focus on the element silicon (Si) at all, but actively extracts silicon (Si). It wasn't something to do. In other words, the invention was not aimed at obtaining a silicon compound.
  • Patent Document 4 describes a method for producing a silicate having a specific molar ratio by reacting rice husk ash with a silicate precursor.
  • Patent Document 4 also uses rice husk ash as a raw material (claim 1 of Patent Document 4, etc.), and there is no mention of the technical concept of extracting water-soluble silicon compounds present in rice husks. There's no suggestion.
  • Patent Document 5 discloses that a raw material is produced by mixing silica ash obtained by burning rice husks so that the C/Si molar ratio is 0.2 or more and 2.0 or less, and the raw material is injected with an inert gas. A manufacturing method is described in which the raw material is heated by irradiation with microwaves in an atmosphere, and silica is reduced to obtain metallic silicon. However, in Patent Document 5, silica ash obtained by burning rice husks is obtained and used as a raw material (Claim 1, [0050] Example 1, etc. of Patent Document 5).
  • silicon dioxide which is a silicon-containing substance, exists mainly in rocks as quartz, and among them, large transparent crystals are called quartz, and sand-like ones are called silica sand, and are used for various purposes. has been done. Furthermore, quartz glass obtained by heating silicon dioxide at high temperature and once melting it is also used for various purposes.
  • Patent Document 3 which does not focus on silicon (Si) at all, all prior art techniques involve burning rice husks in the air and turning them into ash, and converting water-insoluble inorganic substances such as silicon dioxide (SiO 2 ) into It is then used as a raw material (for extraction, etc.).
  • the raw material rice husks are burned, There was no idea to extract silicon (Si) without destroying its form as a water-soluble substance originally contained in a plant-derived material called rice husk.
  • the present invention has been made in view of the above-mentioned background art, and the object is to easily and efficiently use a specific part of a specific plant as a raw material instead of using silicon dioxide contained in rocks, sand, etc. as a raw material.
  • a manufacturing method for obtaining an aqueous silicon compound solution, a water-soluble silicon compound, and an "aqueous silicon compound solution” having specific uses with low energy and the above-mentioned "aqueous silicon compound solution” produced by the manufacturing method. be.
  • silicon compound aqueous solutions and water-soluble silicon compounds can be produced simply, efficiently, and with low energy by using rice husks as a raw material and producing them using a specific method. Furthermore, it has been found that various silicon compounds can be obtained at extremely low total cost starting from rice husks using the silicon compound aqueous solution as a raw material.
  • the present invention is a method for producing an aqueous silicon compound solution that is applicable to uses other than those that utilize the effects of natural organic substances contained in rice husk, Using the rice husk as an object to be extracted without subjecting it to an oxidation reaction in the presence of oxygen, without performing a step of producing silicon dioxide, and without carbonizing the rice husk, with water at a temperature of 20° C. or higher and 180° C. or lower,
  • the present invention provides a method for producing an aqueous silicon compound solution, characterized in that the silicon (Si) element in the extraction target is extracted into water in the form of a water-soluble silicon compound already present in the rice husk.
  • the present invention also provides a method for producing the silicon compound aqueous solution, wherein the extraction target is rice husk, which is neither rice husk ash nor smoky charcoal derived from rice husk.
  • the present invention provides a method for producing the aqueous solution of silicon compounds, which extracts the water-soluble silicon compounds contained in untreated rice husks while maintaining their original chemical structure without causing any chemical changes. be.
  • the present invention provides the above silicon compound aqueous solution extracted such that the concentration of the water-soluble silicon compound is 20 mass ppm or more in terms of silicon atom content with respect to the entire silicon compound aqueous solution immediately after extraction.
  • the present invention provides a method for manufacturing.
  • the present invention involves removing lignin and/or coloring components or rice husk odor components contained in rice husks, and then extracting the rice husks using fresh water at a temperature of 20°C or higher and 180°C or lower.
  • the present invention provides a method for producing the silicon compound aqueous solution, which comprises removing the silicon compound aqueous solution from the obtained silicon compound aqueous solution.
  • the present invention is characterized in that the aqueous silicon compound solution produced by the above-described method for producing an aqueous silicon compound solution is used, and the aqueous silicon compound solution is produced while maintaining the chemical structure that exhibits the water solubility of the silicon compound in the aqueous silicon compound solution.
  • the present invention provides a method for producing a water-soluble silicon compound-containing food or drink.
  • the present invention also provides a method for producing an agent for preventing and improving muscle, blood vessel, or bone disorders, which is characterized by using the above-described method for producing a water-soluble silicon compound-containing food or drink.
  • the present invention also provides an aqueous silicon compound solution produced by the method for producing an aqueous silicon compound solution described above.
  • the present invention is characterized in that it contains an aqueous silicon compound solution produced by the method for producing an aqueous silicon compound solution according to the above claims, or a concentrate obtained by distilling off water from the aqueous silicon compound solution.
  • the present invention provides silicon compound-containing food and drink products.
  • the present invention also provides an agent for preventing and improving muscle, blood vessel, or bone disorders, which is produced by the above-described method for preventing and improving muscle, blood vessel, or bone disorders. .
  • the silicon (Si) element in the rice husk is extracted into water in the form of water-soluble silicon compounds already present in the rice husk.
  • Acquiring elements is efficient and therefore inexpensive.
  • silicon (Si) element can be extracted using an extremely simple method, resulting in a significant cost reduction. . Since rice husk can be obtained as waste, it does not increase the cost of raw materials compared to "rocks and sand" such as quartz and silica sand.
  • the extracted form is not silicon dioxide (SiO 2 ) but a water-soluble silicon compound (H 2 SiO 3 , H 4 SiO 4 , Si(OH) 4 , condensates thereof, etc.), the water solubility is reduced. For required applications, it can be used almost as is, although it may be concentrated or diluted, so further cost reductions can be expected. Furthermore, since it is extracted in the form of a water-soluble silicon compound, it is easy to convert the chemical structure into "elementary silicon or silicon-containing substances (other silicon compounds)".
  • the use of the silicon compound aqueous solution of the present invention is to maintain the water solubility of the silicon compound aqueous solution of the present invention, or to maintain the water solubility without chemically changing the water-soluble silicon compound contained in rice husks.
  • Applications where it is used as is is particularly preferred. When used for such purposes, the manufacturing process can be shortened; it is safe because it can be used with the chemical structure contained in the natural product; and it is possible to reduce costs.
  • the silicon (Si) element is extracted from rice husk and the silicon (Si) element (containing compounds) is chemically structured into "elementary silicon and silicon-containing substances (other silicon compounds)" according to various purposes and uses.
  • rice husks are first turned into rice husk ash or smoldering charcoal, that is, once in the form of silicon dioxide (SiO 2 ), etc., and the silicon (Si) element is extracted from there (Patent Document 1, 2, 4, 5, etc.).
  • Silicon (Si) elements are often used as inorganic substances, such as silicon wafers, high-purity semiconductor gases, and metal silicon nanoparticles, and for this purpose, it is sufficient to extract silicon (Si) elements. Therefore, in the past, when using rice husks as a raw material, it was considered that they were first burned to remove unnecessary organic matter. In fact, when attempting to separate silicon (Si) from a substance or perform its qualitative or quantitative analysis, it is usually incinerated in a platinum crucible or heated at high temperatures using atomic absorption.
  • rice, wheat, etc. absorb water-soluble silicon compounds such as silicic acid (salts) from their roots to the rice husk, transport them, and accumulate them in the rice husk.
  • Water-soluble silicon compounds such as silicic acid exist in an ionized state and are unstable, so rice, wheat, etc. are stabilized by incorporating them into the cuticle layer of rice.
  • to convert silicic acid into silicon dioxide it is necessary to add energy to remove the hydroxyl groups and crystallize it.
  • a silicon compound aqueous solution containing an unexpectedly high concentration of silicon (Si) element can be easily obtained in large quantities by extraction with water.
  • silicon compounds with bonded hydroxyl groups can be made from minerals, but this requires cutting down mountains to create mines, pulverizing the resulting minerals, and repeatedly smelting them at high heat of over 2000 degrees Celsius. Because it is produced through chemical industrial processes such as refining, it has low energy efficiency and is not suitable for the current era of recycling-based methods that aim to reduce energy loads.
  • the method for producing an aqueous silicon compound solution of the present invention that is, if it is extracted from rice husks with water, the resulting product is water-soluble, so it can be easily ingested by humans and livestock as it is, and the intake efficiency is high. (There are no problems in body dynamics) and the manufacturing method is simple, so it has a high matching property and is extremely useful as a silicon compound-containing food or drink. It goes without saying that it is more effective for animals (including humans) to ingest the water-soluble silicon compound of the present invention than to ingest something poorly soluble in water such as silicon dioxide (SiO 2 ). Furthermore, since the silicon compound aqueous solution of the present invention is derived from plants, it is highly safe and can be ingested with confidence, making it optimal as a food raw material.
  • the obtained silicon compound aqueous solution if water is distilled off and concentrated from the obtained silicon compound aqueous solution, or if food-grade powder is added to the obtained silicon compound aqueous solution and powdered, it can be used as a gel-like or solid food or drink product. It is useful and can suitably compensate for the lack of silicon in the body.
  • a silicon compound-containing food or drink containing "a silicon compound aqueous solution produced by the method for producing a silicon compound aqueous solution of the present invention” or "a concentrate obtained by distilling water off from the silicon compound aqueous solution” is Since the compound is water-soluble, it is advantageous in terms of the number of manufacturing steps and manufacturing cost, and because it is a natural product (origin), it is safe in the body and may have good pharmacokinetics.
  • Rice husks are produced in large quantities, and it is difficult to dispose of them as waste.
  • the present invention not only has the above-mentioned excellent effects, but also provides excellent waste treatment effects.
  • rice husk, which is the raw material for extraction is easy to obtain and secure, and the raw material cost is low, so the total manufacturing cost can be kept low.
  • the method for producing an aqueous silicon compound solution of the present invention is a method for producing an aqueous silicon compound solution that is applicable to uses other than those utilizing the effects of natural organic substances contained in rice husks, and includes: Using the rice husk as an object to be extracted without subjecting it to an oxidation reaction in the presence of oxygen, without performing a step of producing silicon dioxide, and without carbonizing the rice husk, with water at a temperature of 20° C. or higher and 180° C. or lower, The method is characterized in that the silicon (Si) element in the extraction target is extracted into water in the form of a water-soluble silicon compound already present in the rice husk.
  • the "rice husk” in the present invention may be the residue after removing brown rice (bran and white rice), that is, it may be after threshing and hulling, and the starting material (raw material) in the present invention is the rice husk. It may contain other things as long as it contains.
  • the rice husk is not limited to rice husk, but may be wheat husk such as barley or wheat.
  • the rice husk is not limited to the husk of glutinous rice (glutinous rice), but may be the husk of glutinous rice (glutinous rice) or the like. Examples of the rice husk include rice husks of Japonica (Japanese-type rice), Indica (Indian-type rice), and Javanica (Java-type rice).
  • Rice husk consists of the outermost layer, the cuticula layer, and the inner layer of cellulose, hemicellulose, and lignin, and silicon (Si) is mainly contained in the cuticle layer.
  • the object to be immersed in water and heated may be the entire rice husk, or only the ⁇ cuticular layer containing silicon compounds'' from which ⁇ cellulose, hemicellulose, and lignin layers'' have been removed. ⁇ Since it is costly or difficult to remove the hemicellulose/lignin layer in advance, it is preferable to use the entire rice husk.
  • Rice husks may be crushed before extraction, but since silicon (Si) is mainly contained in the "surface layer of the cuticle layer", crushing is not effective. Furthermore, considering cost, it is preferable not to (substantially) crush the rice husks.
  • Lignin and/or coloring components or rice husk odor components contained in rice husk usually degrade the quality of the silicon compound aqueous solution of the present invention.
  • lignin etc. contains in rice husk usually degrade the quality of the silicon compound aqueous solution of the present invention.
  • lignin, cellulose, etc. are hydrolyzed using acids such as sulfuric acid; solvents such as water, ethanol, phenol, etc., and the molecular weight of lignin, cellulose, etc. is reduced and water solubilized.
  • acids such as sulfuric acid
  • solvents such as water, ethanol, phenol, etc.
  • lignin and the like An example of this is to remove lignin and the like in advance.
  • lignin can be removed in advance by reducing the molecular weight of lignin, making it water-soluble, etc. using hot water or steam at 80°C or higher, superheated steam at 100°C or higher, or high-pressure hot water at 100°C or higher. preferable.
  • rice husks On the outside, rice husks have a cuticle layer that contains silicon compounds, enzymes such as cutinase, cutin (a polymer of unsaturated fatty acids), and wax (a water-insoluble fatty acid ester). It consists of a cuticle layer) and a ⁇ cellulose, hemicellulose, and lignin layer'' that exists inside the cuticle layer. Furthermore, a bran layer and polished rice are present further inside the rice husk.
  • enzymes such as cutinase, cutin (a polymer of unsaturated fatty acids), and wax (a water-insoluble fatty acid ester). It consists of a cuticle layer) and a ⁇ cellulose, hemicellulose, and lignin layer'' that exists inside the cuticle layer.
  • a bran layer and polished rice are present further inside the rice husk.
  • Silicon compounds are abundantly contained in the cuticle layer of rice husks, so they are preliminarily contained in the "cellulose/hemicellulose/lignin layer", lignin, and/or coloring components or rice husk odor components, and/or the above-mentioned silicon (Si). It is also preferred to remove the uncontained substances by a method other than combustion and then extract the rice husks with additional fresh water.
  • the silicon compound aqueous solution obtained by the production method of the present invention is used for silicon compound-containing foods and drinks, it is also preferable to remove the above-mentioned substances.
  • the method in addition to the above-mentioned “removal by a method other than combustion", it is preferable to "remove by a method other than strong acid or strong alkali treatment".
  • lignin is present in the resulting silicon compound aqueous solution. It contains (organic) impurities such as cellulose (derived materials), so they are removed. Methods for removal include membrane separation, adsorption separation on activated carbon, etc., chromatographic separation using gel, etc., which will be described later.
  • the above (2) is more preferable than the above (1) in terms of difficulty, cost, etc.
  • the present invention is a method for producing an aqueous silicon compound solution that is applicable to uses other than those utilizing the effects of natural organic substances contained in rice husks.
  • the present invention is a method for producing an aqueous silicon compound solution that is applied to uses that utilize the "effects and efficacy of water-soluble silicon compounds" contained in rice husks. If you want to extract organic substances such as lignin from rice husks, it is natural to do so without burning them.
  • the present invention uses a different extract and has a completely different technical idea.
  • the rice husk used as a raw material in the present invention has not been subjected to an oxidation reaction such as combustion in the presence of oxygen, that is, has not undergone a process of producing silicon dioxide (SiO 2 ).
  • the object to be extracted in the present invention is rice husk, which is neither rice husk ash nor smoky charcoal derived from rice husk.
  • the extraction target in the present invention is rice husk that has not been ashed or carbonized.
  • rice husks are burned to produce rice husk ash or smoked charcoal, and then converted to silicon dioxide (SiO 2 ), which uses silicon dioxide (SiO 2 ) in rocks such as quartz or sand such as silica sand as a raw material.
  • SiO 2 silicon dioxide
  • this method is disadvantageous in all respects.
  • water-insoluble silica sicon dioxide (SiO 2 )
  • SiO 2 water-insoluble silica
  • lignin and/or coloring components or rice husk odor components contained in rice husks it is preferable to remove lignin and/or coloring components or rice husk odor components contained in rice husks, but if carbonized, the above-mentioned "organic substances contained in rice husks" In some cases, it may not be possible to completely remove carbon. Furthermore, elemental carbon (C) may interfere with the extraction of water-soluble silicon compounds.
  • the production method of the present invention is characterized in that the silicon compound is extracted using water at a temperature of 20° C. or higher and 180° C. or lower.
  • the lower limit of the water temperature is preferably 40°C or higher, more preferably 60°C or higher, even more preferably 80°C or higher, and particularly preferably boiling water at 100°C under normal pressure. It is particularly preferable to use boiling water that is boiling at 100° C., since there is no need to control the temperature and extraction can be carried out stably at high temperatures. If the temperature is too low, the extraction efficiency may deteriorate or the extraction time may become longer.
  • the upper limit of the water temperature is essentially 180°C or lower, preferably 160°C or lower, more preferably 140°C or lower, even more preferably 120°C or lower, and particularly preferably 100°C or lower.
  • Water above 100°C is obtained by preventing boiling by applying pressure.
  • water here may be any liquid having the chemical formula H 2 O, and includes, for example, so-called hot water, hot water, and the like.
  • the temperature is too high, the high temperature may be wasted; organic substances in the rice husks may be decomposed, making subsequent purification (removal of impurities from the obtained silicon compound aqueous solution) difficult.
  • the decomposition of cellulose in rice husks may be accelerated, making purification inefficient.
  • water becomes subcritical water, which accelerates the decomposition of organic matter in the rice husks, making subsequent purification difficult.
  • the concentration of (organic) impurities in the resulting silicon compound aqueous solution may increase. .
  • the pressure during extraction is not particularly limited as long as water at the above temperature can be produced, but it is particularly preferable that the extraction temperature is 100°C or less, and normal pressure (1 atm) is recommended to reduce production costs. It is also preferable from this point of view. High pressures may complicate the equipment.
  • the water (extracted water) used in the present invention is preferably substantially neutral water.
  • substantially neutral refers to a pH of 5.7 to 8.3, preferably a pH of 6 to 8, particularly preferably a pH of 6.5 to 7.5.
  • the compound includes, but is not particularly limited to, a pH adjuster; a compound that decomposes cuticle or cellulose; a compound that decomposes protein; and the like.
  • alkaline substances such as sodium hydroxide, calcium hydroxide, sodium (hydrogen) carbonate, and ammonia are blended in the extracted water, calcium silicate, sodium silicate, ammonium silicate, etc. are generated. In the present invention, if these are not produced and the entire composition is made up of only plant-derived substances, it is particularly suitable for the food field.
  • the method for producing an aqueous silicon compound solution of the present invention is characterized in that the silicon (Si) element in the extraction target is extracted into water in the form of a water-soluble silicon compound already present in the rice husk, which is the extraction target. do.
  • “Already present in rice husk” means that it is present in raw or dried rice husk, and it can be burned, oxidized, or carbonized to produce silicon dioxide (SiO 2 ), etc. This means that it does not become water-insoluble.
  • the water-soluble silicon compounds contained in the rice husk while maintaining its original chemical structure without causing any chemical changes. It is preferable to produce the silicon compound while maintaining the chemical structure that makes the silicon compound water-soluble in the silicon compound aqueous solution.
  • the obtained silicon compound aqueous solution may be diluted or concentrated before use. It has the following effects: ⁇ natural products can be used as they are'' in foods and drinks.
  • Substances that rice and wheat transport from their roots to the rice husk must be water-soluble, as they cannot be transported to the rice husk if they are in granular form and are not dissolved in water. Also, the silicon compounds stored in rice husks should be water-soluble.
  • the present invention is characterized in that the water-soluble substance is extracted with water while maintaining its water solubility.
  • compositional formula of the water-soluble silicon compounds already present in rice husks has not been completely specified, but at least they are silicic acid (compositional formula: H 2 SiO 3 ) or silicic acid. It has been confirmed that some substances are contained in the form of acid ions (compositional formula: SiO 3 2- ).
  • the chemical structure of the water-soluble silicic acid compound in the silicon compound aqueous solution of the present invention is not particularly limited. For example, it can also be written as Si(OH) 4 .
  • the concentration of the water-soluble silicon compound in the present invention it is preferable to extract the water-soluble silicon compound so that the concentration thereof is 20 mass ppm or more in terms of silicon atom content, based on the entire silicon compound aqueous solution immediately after extraction. Immediately after extraction, it is desirable to extract the amount to preferably 30 mass ppm or more, more preferably 45 mass ppm or more, still more preferably 60 mass ppm or more, particularly preferably 75 mass ppm or more.
  • the method for producing a silicon compound aqueous solution of the present invention it is possible to extract the silicon compound aqueous solution to the above mass ppm or more with respect to the entire silicon compound aqueous solution, and the later processing is easier when obtained at a high concentration. This is preferable because it is flexible and flexible.
  • the upper limit is not particularly limited as long as it can be extracted, but it is preferable to extract so that the content of silicon atoms is 2000 mass ppm or less in terms of the entire silicon compound aqueous solution immediately after extraction, and 1500 mass ppm or less. It is more preferable to extract so that the amount is less than ppm, and it is particularly preferable to extract so that the amount is less than 1000 ppm by mass. If the above upper limit is too high, in the case of batch-type extraction; as the concentration increases, the extraction rate decreases; if high temperature is used to obtain a high concentration, hydrolysis of cellulose, etc. in rice husks may be accelerated. , when subsequent purification becomes difficult; when there is no need to increase the concentration to such a high level, etc.
  • rice husk is first immersed in water, and the mass ratio of "rice husk” and “water” at that time is such that water-soluble silicon compounds can be suitably extracted and the concentration as silicon (Si)
  • water is preferably 5.0 to 1000 parts by mass, more preferably 10 to 700 parts by mass, and 20 to 1000 parts by mass per 1.0 parts by mass of rice husks. More preferably 500 parts by weight, particularly preferably 50 to 300 parts by weight.
  • the water may be reduced by evaporation, but the above range is the mass ratio of "rice husk” to "water” at the initial stage of extraction or at the time of preparation.
  • the silicon (Si) concentration in the silicon compound aqueous solution obtained will be low; the volume will become too large, making subsequent handling such as concentration difficult; in the first place, that amount of water is not required; Water is wasted; equipment becomes unnecessarily large and costs increase; etc.
  • the extraction efficiency of silicon (Si) is extremely high. A high silicon compound aqueous solution can be produced.
  • the present invention is characterized in that an aqueous solution containing a high concentration of silicon compounds is obtained by extraction.
  • the water-soluble silicon compound contained in the silicon compound aqueous solution of the present invention contains many metasilicate ions. Therefore, assuming that the above content in terms of silicon atoms is entirely contained in metasilicate ions (SiO 3 2- ), in the present invention, the content of silicon atoms is extracted to be 20 mass ppm or more. is preferable (because it can be extracted), that is, an aqueous metasilicate ion solution containing metasilicate ions (SiO 3 2 ⁇ ) of 54 mass ppm or more can be obtained.
  • the metasilicate ion (SiO 3 2- ) contained in the silicon compound aqueous solution of the present invention is preferably 100 mass ppm or more (100 mass ppm or more is obtained), and more preferably 150 mass ppm or more (150 mass ppm or more is obtained). 200 mass ppm or more is more preferable (200 mass ppm or more is obtained), and particularly preferably 250 mass ppm or more (250 mass ppm or more is obtained).
  • the upper limit of the silicon compound content in the silicon compound aqueous solution of the present invention converted into "silicon atom content" and the upper limit of the metasilicate ion (SiO 3 2- ) contained in the silicon compound aqueous solution of the present invention is not particularly limited, but it will gel if it reaches a very high concentration. Therefore, the upper limit is the concentration at which gelation does not occur.
  • the method for quantifying silicon (Si) is not particularly limited, and any quantitative analysis method may be used. Alternatively, it may be quantified as metasilicate ion (SiO 3 2- ) or the like and converted into the content ratio (mass ppm) of silicon (Si). Examples of such "methods for quantifying silicate ions (SiO 3 2- )" include the molybdenum blue colorimetric method.
  • the value of the silicon (Si) content of the present invention is determined by quantifying silicate ions (SiO 3 2- ) using a molybdenum blue colorimetric method and converting it into a silicon (Si) content ratio (mass ppm).
  • the "silicon content” in the present invention is defined as the value obtained by such a method.
  • Such a device include, for example, Pack Test (registered trademark) (model: WAK-SiO 2 , manufactured by Kyoritsu Physical and Chemical Research Institute, Inc.).
  • the silicon compound aqueous solution of the present invention may contain substances other than water-soluble silicon compounds, such as lignin, cutinase, cutin, wax, cellulose, hemicellulose, starch, etc. in rice husks. Can be mentioned.
  • the above components, coloring components, odor components, unpleasant components, etc. in rice husks, for example, especially when used in foods and drinks, etc. should be contained below the permissible amount, or should not be contained as much as possible. It is preferable because it prevents coloring and becomes colorless and transparent; it removes bitterness and harshness to make it delicious or tasteless; it removes the odor peculiar to rice husk; and so on.
  • the present invention also provides a silicon compound aqueous solution produced by the above-mentioned "method for producing a silicon compound aqueous solution.”
  • the concentration of the silicon compound aqueous solution in the present invention may be adjusted to an appropriate value for the intended use by concentrating or diluting it with water, and is not particularly limited.
  • the atomic content is preferably 0.1 mass ppm or more and 1000 mass ppm or less, more preferably 1.0 mass ppm or more and 300 mass ppm or less, and particularly preferably 3 mass ppm or more and 100 mass ppm or less. Within the above range, the concentration is suitable for a wide range of applications.
  • aqueous solution in silicon compound aqueous solutions, etc. includes those that have been increased in concentration to have a high viscosity, and gel-like solutions that contain water.
  • concentration includes not only those that have been made highly concentrated to have a high viscosity, but also gel-like products containing water and powder-like products. Even if this happens, diluting with water may result in an aqueous solution with a low viscosity, or there may be parts where the viscosity becomes an aqueous solution.
  • gel form there is a high possibility that it will be absorbed by the body, and there are food forms such as jelly, which have a wide range of applications, so there are actually positive uses for it.
  • the silicon compound aqueous solution obtained by the production method of the present invention contains silicon (Si) at least as metasilicate ions (SiO 3 2- ), but silicon (Si) is contained either as orthosilicate ions, metasilicate ions, or metasilicate ions.
  • the details are not clear, such as whether it is disilicate ions, amorphous silica (SiO 2 ), or whether they are mixed in small amounts, and there is no clear analysis of the silicon compounds contained in the cuticle layer of rice husks. . It is also described as Si(OH) 4 .
  • the aqueous solution may contain trace amounts of cellulose, hemicellulose, lignin, cutinase, cutin, wax, starch, coloring components, odor components, unpleasant taste components, and the like.
  • the silicon compound aqueous solution of the present invention can be used to produce a water-soluble silicon compound-containing food or drink.
  • food and drink includes general food and drink and health food and drink
  • health food and drink includes liquids and solids of all dosage forms.
  • the present invention also provides a method for producing a water-soluble silicon compound-containing food or drink using the aqueous silicon compound solution produced by the above-mentioned "method for producing an aqueous silicon compound solution.” Furthermore, the present invention is characterized in that the silicon compound aqueous solution produced by the above-described method for producing a silicon compound aqueous solution is used, and the silicon compound aqueous solution is produced while maintaining the chemical structure that exhibits the water solubility of the silicon compound in the silicon compound aqueous solution. It is also a method for producing food and drink products containing water-soluble silicon compounds.
  • methods for turning a silicon compound aqueous solution into a water-soluble silicon compound-containing food or drink include, for example, making it into a liquid food or drink as it is; concentrating or diluting the silicon compound aqueous solution; or concentrating and making it into a gel form. Before or after concentration, food-grade powder or the like is added to powder or solid in appearance; additives/compounds or other active ingredients are added.
  • silicon (Si) When rice, wheat, etc. absorb water from the soil, silicon (Si) must be in the form of water-soluble silicon compounds such as silicic acid (salts). Even when stored in the cuticle layer of rice husk, it has the property of being easily dissolved in water, regardless of its chemical structure. According to the production method of the present invention, the content of water-soluble silicon compounds can be increased, and food and drink products with a high content of elemental silicon (Si) can be obtained very easily and efficiently.
  • water-soluble silicon compounds such as silicic acid (salts).
  • an aqueous solution with a surprisingly high content of silicon (Si) can be obtained with a (relatively small amount) of water.
  • the silicon compound-containing foods and drinks obtained by the present invention are easy to ingest, can effectively take silicon (Si) into the body, and have good pharmacokinetics.
  • the present invention also provides a silicon compound-containing food or drink, which is produced by the "method for producing a silicon compound-containing food or drink” of the present invention.
  • the silicon (Si) content concentration of the silicon compound-containing food or drink can be changed as appropriate depending on the food or drink produced therefrom. That is, the liquid obtained by the "method for producing an aqueous silicon compound solution” of the present invention can be diluted or concentrated to produce a silicon compound-containing food or drink. Therefore, the present invention is characterized by containing an "aqueous silicon compound solution produced by the method for producing an aqueous silicon compound solution of the present invention" or "a concentrate obtained by distilling water off from the aqueous silicon compound solution". It is also a food and drink product containing silicon compounds.
  • the present invention also includes silicon compound-containing foods and drinks that are diluted with water to form an aqueous solution with a concentration lower than that at the time of extraction.
  • the above-mentioned general food and beverages are not particularly limited, and specifically include, for example, drinking water; juices such as fruit juice (fruit juice) and vegetable juice; and (soybean) dairy products such as milk, soy milk, yogurt, and milk drinks. or fermented foods and drinks; seasonings such as sauces, soy sauce, mayonnaise, ketchup, and dressings; all dishes that use water such as simmered foods, boiled foods, soups, rice, noodles, rice cakes, and pickles; and the like.
  • juices such as fruit juice (fruit juice) and vegetable juice
  • dairy products such as milk, soy milk, yogurt, and milk drinks. or fermented foods and drinks
  • seasonings such as sauces, soy sauce, mayonnaise, ketchup, and dressings
  • all dishes that use water such as simmered foods, boiled foods, soups, rice, noodles, rice cakes, and pickles; and the like.
  • the silicon compound aqueous solution of the present invention is used as water for cooking such as boiled foods, boiled foods, and soups.
  • the silicon compound aqueous solution of the present invention is used as water for kneading and cooking.
  • the silicon compound aqueous solution of the present invention is used as water for pickling liquid such as bran bran.
  • the above-mentioned health foods and drinks include, but are not particularly limited to, liquid preparations, syrup preparations, tablets, capsules, gel preparations, preparations made by incorporating an aqueous silicon compound solution into food grade powder, etc., to form a powder or solid. .
  • the silicon compound aqueous solution and the silicon compound-containing food and drink of the present invention are adjusted to an amount of 50 mg/day of silicic acid for athletes who have chronic muscle pain due to muscle strain, and are given daily for 7 days. When I received it, I actually saw some relief from my symptoms. Furthermore, the silicon compound aqueous solution and the silicon compound-containing food and drink products of the present invention were actually found to be effective in improving blood vessel and bone disorders.
  • the present invention also provides a method for producing an agent for preventing and improving disorders of muscles, blood vessels, or bones, which is characterized by using the above-mentioned method for producing a water-soluble silicon compound-containing food or drink, and a product produced by the method. It is also an agent for preventing and improving disorders of muscles, blood vessels, or bones.
  • the silicon compound contained in the silicon compound aqueous solution in the present invention is water-soluble, it can be ingested as it is or by simply diluting or concentrating it without any chemical reaction, which is convenient and can reduce costs. Moreover, when ingested, silicon (Si) can be effectively taken into the body, and the above-mentioned effects are suitably exerted.
  • a lotion made of the silicon compound aqueous solution of the present invention as it is or diluted with water does not contain "substances that have moisturizing properties in themselves” such as glycerin, but is effective against skin irritation. It showed “high moisturizing properties”. Furthermore, the cosmetic containing the silicon compound aqueous solution of the present invention exhibited "high moisturizing properties for the skin” even if it did not contain "substances that themselves have moisturizing properties” such as glycerin and oily components.
  • the present invention is characterized by using an aqueous silicon compound solution produced by the above-described method for producing an aqueous silicon compound solution, while maintaining the chemical structure that makes the silicon compound in the aqueous silicon compound solution exhibit water solubility. It is also a method for producing a cosmetic, and a cosmetic characterized by being produced by the production method.
  • the present invention is characterized in that the aqueous silicon compound solution produced by the above-described method for producing an aqueous silicon compound solution is used, and the aqueous silicon compound solution is produced while maintaining the chemical structure that exhibits the water solubility of the silicon compound in the aqueous silicon compound solution. It is also a method for producing a lotion, and a lotion characterized by being produced by the method. Among cosmetics, the aspect of the lotion is preferable because it contains a large amount of water and almost no oily components, and therefore it is easy to exhibit the above-mentioned effects of the silicon compound aqueous solution of the present invention.
  • the silicon compound contained in the silicon compound aqueous solution in the present invention is water-soluble, it can be applied to the skin as it is or just by diluting it without any chemical reaction, so it is easy to exhibit the above-mentioned effects, and it is simple and cost-reduced. . Moreover, when ingested, silicon (Si) can be effectively taken in through the skin, and the above-mentioned effects are suitably exhibited.
  • the silicon compound aqueous solution of the present invention can be suitably used for food and drink products, but because of its high acquisition efficiency of silicon (Si) element, it can also be used for producing elemental silicon or silicon-containing products. That is, although elemental silicon or silicon-containing substances were conventionally obtained from silicon dioxide (SiO 2 ) in rocks or sand, they can be obtained from the silicon compound aqueous solution of the present invention.
  • the present invention uses an aqueous silicon compound solution produced by the above method for producing an aqueous silicon compound solution to produce siloxane, white gelled silicic acid (H 2 SiO 3 ), silica gel (SiO 2 .mH 2 O (m is natural number)), silicate (M n SiO 3 (M is a monovalent or divalent metal, n is 2 or 1)), silicon dioxide (SiO 2 ), silanol, fluorosilicic acid (H 2 SiF 6 ), Alkoxysilane, alkylalkoxysilane (R m Si(OR') 4-m ) (R, R' are alkyl groups, m is 1, 2 or 3), silicon tetrachloride (SiCl 4 ), or elemental silicon (Si ) is also a method for producing elemental silicon or silicon-containing products.
  • white gelled silicic acid H 2 SiO 3
  • silica gel SiO 2 .mH 2 O (m is natural number)
  • Example 1 After washing 30 g of rice husk after threshing with pure water, it was immersed in 1000 mL of purified water in a heat-resistant glass bottle, and treated in an autoclave at 121° C. and 1.1 atm for 15 minutes.
  • Silicon compounds accumulated in the rice husks were eluted into water as silicate ions by treatment at 121° C. and 1.1 atm for 15 minutes to form an aqueous solution (extract).
  • This aqueous solution (extract) can be used as a silicon compound-containing food or drink.
  • Si silicate ions
  • the silicon compound-containing food and drink obtained above By drinking the silicon compound-containing food and drink obtained above, the silicon compound could be ingested into the body. Although it was slightly yellow in color, the taste and odor when consumed were completely acceptable as, for example, a health food. Furthermore, the level was acceptable for general foods, and when mixed with other beverages such as tea, juice, coffee, milk, soy milk, cocoa, etc., it became more suitable as general foods (or health foods).
  • Example 2 In Example 1, after autoclave treatment under the above conditions (after heat treatment under the same conditions), the resulting aqueous solution was extracted, new purified water was added thereto, and autoclave treatment under the same conditions (after heat treatment under the same conditions) was performed. ) was repeated four times.
  • the silicate ion (SiO 3 2 ⁇ ) concentration was 200 ppm or more. That is, even the fourth silicon compound-containing food/beverage product after repeating the above treatment four times showed a silicon (Si) atom concentration of 74 mass ppm or more.
  • Example 3 In Example 2, the first to third elutions of "unnecessary compounds such as lignin" were replaced with "121 ° C., 1.1 atm, 15 minutes” using an autoclave as described in Examples 1 and 2. The extraction was carried out at 98° C. and 1 atm (normal pressure) for 15 minutes using a general-purpose hot water extraction device designed to be used at normal pressure. The fourth extraction was performed under the extraction conditions described in Examples 1 and 2: "121°C, 1.1 atm, 15 minutes.” Other than that, the same procedure as in Example 1 was carried out.
  • Example 2 When the obtained silicon compound-containing food and drink products were evaluated, the same evaluation results as in Example 2 were obtained. Even if ⁇ unnecessary compounds such as lignin'' are eluted and removed by normal hot water extraction at 100°C or less, if you do it first (in advance), you can remove the unpleasant husk while maintaining the silicon content. It was found that the odor can be eliminated and the taste, flavor, and appearance (coloring) are improved.
  • Example 4 When the temperature of Example 1 was increased (changed) from 121°C to 130°C and autoclave treatment was carried out in the same manner as in Example 1, 200 mass ppm or more of silicate ions (SiO 3 2 - ) concentration, that is, the silicon atom concentration was 74 mass ppm or more. By raising the processing temperature, the characteristic odor of rice husks disappeared, making it more useful as drinking water and food and drink.
  • silicate ions SiO 3 2 -
  • Example 5 a silicon compound-containing food and drink product was produced in the same manner as in Example 1, except that 30 g of "superheated steam-treated rice husk" which had been previously treated as described below was used instead of "30 g of rice husk". That is, 50 g of rice husks were placed in a superheated steam oven with the upper heater set at 300°C and the lower heater set at 300°C, superheated steam at 280°C was introduced, and the rice husks were placed in an atmosphere of superheated steam at that temperature for 2 minutes and 30 seconds. exposed. After this treatment, heat treatment was performed in the same manner as in Example 1 using 30 g of "superheated steam-treated rice husks".
  • Example 6 In Example 1, instead of using an autoclave and treating at 121°C and 1.1 atm for 15 minutes, a general-purpose hot water extraction device designed to be used at normal pressure was used to perform the treatment at 100°C and 1 atm. Hot water extraction was carried out for 15 minutes and 90 minutes, respectively (normal pressure).
  • Example 7 A heat-resistant container was charged with 1000 mL of pure water and 5.0 g of rice husks and sealed. The mixture was placed in an autoclave and heated at 121° C. for 15 minutes, and the water-soluble silicon compound was extracted into water to obtain an aqueous silicon compound solution.
  • the concentration of silicon (Si) atoms in the obtained silicon compound aqueous solution was determined by the same method as in Example 1, and was found to be 500 mass ppm.
  • Example 8 1000 mL of water and 5.0 g of rice husks were put into a 2 L beaker, and after boiling at 100° C., the mixture was further boiled for 10 minutes to obtain an aqueous silicon compound solution.
  • the concentration of silicon (Si) atoms in the obtained silicon compound aqueous solution was determined by the same method as in Example 1, and was found to be 100 mass ppm.
  • Example 9 Rice husk suspension water having a concentration of [5.0 g of rice husks]/[1 L of water] was placed in a tubular heat exchanger heated to 80° C. with steam, and was allowed to pass through for 3 minutes.
  • the concentration of silicon (Si) atoms in the silicon compound aqueous solution obtained in the above extraction process was determined by the same method as in Example 1, and was found to be 80 mass ppm.
  • Example 10 "Rice husk suspension water” in which rice husks were suspended in water at a concentration of [5.0 g of rice husks]/[1 L of water] was placed in a hot water cooker, and the mixture was allowed to stand at 85° C. for 15 minutes.
  • the concentration of silicon (Si) atoms in the silicon compound aqueous solution obtained above was determined by the same method as in Example 1, and was found to be 80 mass ppm.
  • Yogurt containing silicon compounds was prepared by mixing the silicon compound aqueous solution obtained in Example 8 with milk, adding an appropriate amount of lactic acid bacteria collected and cultured from commercially available yogurt, and leaving to stand.
  • Example 12 ⁇ Application to general foods> When the silicon compound aqueous solutions obtained in Examples 1 to 10 were diluted 10 times and drunk, they were not colored and had no problems in taste or flavor (same as pure water) and were delicious. It has been found that silicon (Si) can be ingested easily and tastefully.
  • Example 13 ⁇ Application to health foods> 5 g of indigestible dextrin was dissolved in 100 mL of each of the silicon compound aqueous solutions produced in Examples 1 to 10, and boiled down in a container to evaporate water to powder the silicon compound-containing food and drink.
  • the obtained powdered silicon compound-containing food or drink could be suitably ingested as it is (as a powder) or in the form of tablets, capsules, or decoction foods.
  • silicon compounds silicon (silicon (Si)) could be easily ingested as a health food.
  • Example 14 ⁇ Application to preventive improvement agent for muscle, blood vessel or bone disorders>
  • the silicon compound aqueous solution of the present invention and the silicon compound-containing food and drink were administered to athletes who had severe muscle pain that was thought to be due to slight muscle strain and had not been chronically cured for a long time. When the concentration was adjusted so that it could be ingested and the patients took it every day for 7 days, it was found that it alleviated muscle pain. It was suggested that it made some contribution to the composition of muscle components. Furthermore, the silicon compound aqueous solution and the silicon compound-containing food and drink products of the present invention were also found to be effective in improving blood vessel and bone disorders.
  • Example 15 ⁇ Application to lotion (improving moisturizing properties)> A silicon compound aqueous solution produced in the same manner as in Examples 1 to 10 was diluted 20 times with distilled water to produce a lotion. The concentration of silicon (Si) atoms in the silicon compound aqueous solution used was determined in the same manner as in Example 1, and was found to be 400 ppm by mass. Therefore, the lotion contained 20 mass ppm of silicon (Si) mainly as silicic acid.
  • the lotion obtained above was distributed to 340 people, and evaluation results were received from 62 of them. The results are shown below as a percentage of the total number of people (62 people).
  • Example 16 A silicon compound aqueous solution produced in the same manner as in Examples 1 to 10 was diluted 20 times with distilled water to produce a lotion. Similar to Example 15, the lotion contained 20 mass ppm of silicon (Si) mainly as silicic acid.
  • Answer 5 I had noticeable skin problems such as dry skin and sensitive skin, but they have clearly improved.
  • Answer 4 I had skin problems such as dry skin and sensitive skin, but they have improved.
  • Answer 3 Did you have any skin problems such as dry or sensitive skin, or if you did, it improved somewhat?
  • Answer 2 I had skin problems such as dry skin and sensitive skin, but they did not improve much.
  • Answer 1 I had skin problems such as dry skin and sensitive skin, but they did not improve.
  • the lotion obtained above was distributed to 340 people, including those with no abnormal skin condition, those with dry or sensitive skin, or those with skin problems, and evaluation results were obtained from 62 of them. I received it. The results are shown below as a percentage of the total number of people (62 people).
  • silicon Si
  • Si can be easily applied to the skin (absorbed from the skin) without resistance, and has the remarkable effect of fundamentally improving skin problems.
  • the method for producing an aqueous silicon compound solution of the present invention can dissolve a highly concentrated silicon compound in water from a natural product called rice husk, and is water-soluble. Therefore, if you ingest it, you can safely take the silicon (Si) element into your body since it is derived from plants. It is also widely used as a raw material for elemental silicon (Si), inorganic silicon compounds, and organic silicon compounds such as silicon resins in electronic materials, chemical materials, and the like.
  • the present invention can be widely used in the fields of manufacturing and using general foods, health foods, cosmetics, etc., the field of manufacturing and using electronic materials and chemical materials, the agricultural field, etc.

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