RU2789671C2 - Composition for production of hydrogen-enriched water and other products - Google Patents

Abstract

FIELD: chemistry.

SUBSTANCE: invention relates to compositions for the production of hydrogen-enriched water, nutraceuticals, cosmetic products, pharmaceutical preparations and other products. In one of embodiments, the invention relates to a composition, for example a tablet, including magnesium metal, at least one water-soluble acid, and a binder. Magnesium metal and at least one water-soluble acid may be present in amounts sufficient for maintaining pH of less than 7, for example, during a certain period of time after the reaction, and concentration of at least 0.5 mM of H₂ after the reaction in 50 ml of water in a container, for example a closed or open container, for example, at least 0.5 mM of H₂ after the reaction in 100 ml of water or at least 0.5 mM of H₂ after the reaction in 500 ml of water. The composition may also include a lubricant.

EFFECT: obtaining hydrogen-enriched water.

101 cl, 2 tbl, 13 ex

Description

STATE OF THE ART TO which THE INVENTION RELATES

Molecular hydrogen has been found to have potential therapeutic applications in various diseases and injuries. For example, H ₂ has been shown to be useful as a method for reducing wrinkles in the skin ( J. Photochem. Photobiol. B . 2012; 106:24-33), treating atopic dermatitis ( Evid. Based Complement. Alternat. Med . 2013; 2013 :538673) and as a recovery regimen after radiotherapy ( Biochem. J. , 2012, 442(1); 49-56). Hydrogen-enriched water is one of the routes by which molecular hydrogen can be administered to individuals. Conventional electrolytic and non-base metal processes for producing hydrogen-rich water typically provide an alkaline solution with a low concentration of H ₂ .

Creating ready-to-use containers with H ₂ (and thus hydrogen-enriched water) has technical difficulties. Often the equipment used to saturate the water with H ₂ gas in sufficient quantities is both expensive and mostly inefficient. When using H ₂ , it can be dissolved in a maximum concentration of 0.8 mm or 1.6 p. under SATP under Henry's Law. To maintain this H ₂ concentration for any period of time, the container may not have any headspace or the beverage must be supersaturated to allow H ₂ to escape into the headspace to reach equilibrium. Even when there is no free space, the level H ₂ in the container is rapidly reduced to ~ 1 m. and continues to decrease to 0 ppm. depending on sealing technology, headspace and initial concentration, as observed for other commercial products on the market. Some products retain little to no H ₂ by the time they reach consumers. For example, the Japanese government recently evaluated products containing H ₂ and found that most of them lacked a detectable level of H ₂ . (http[[://]]www.kokusen.go.jp/news/data/n-20161215_2.html).

Thus, there is a need for new hydrogen rich water compositions that maximize the concentration of dissolved hydrogen.

SUMMARY OF THE INVENTION

The invention relates to compositions for the production of hydrogen-enriched water, nutraceuticals, cosmetics, pharmaceuticals and other products. In one embodiment, the invention relates to a composition, such as a tablet, comprising magnesium metal, at least one water-soluble acid, and a binder. Metallic magnesium and at least one water-soluble acid may be present in amounts sufficient to maintain a pH less than 7, for example, for a specific period of time after the reaction, and an H ₂ concentration of at least 0.5 mM after the reaction in 50 ml of water. In a container, for example, a closed or open container, for example, at least 0.5 mm H ₂ after a reaction of 100 ml of water or at least 0.5 mm H ₂ after a reaction of 500 ml of water. The composition may also include a lubricant.

In another aspect, the invention relates to a composition comprising magnesium metal, at least one water-soluble acid, and a binder, wherein the at least one water-soluble acid has a water solubility of at least 0.01 g/mL. In certain embodiments, the composition disintegrates in less than 5 minutes, in particular less than 2 minutes. In certain embodiments, the composition produces at least 0.5 mM H ₂ upon contact with 50 ml of water in a container at atmospheric pressure and room temperature, such as at least 0.5 mM H ₂ upon reaction in 100 ml of water, or at least Meres of 0.5 mm H ₂ after a reaction of 500 ml of water. The composition may also include a lubricant.

In certain embodiments of the aspects described above, the composition disintegrates in less than 5 minutes, such as in less than 2 minutes. In certain embodiments, the composition, after disintegration, maintains a pH of less than 7 10 minutes after contact with water and produces at least 0.5 mm H ₂ after contact with 50 ml of water in a container at atmospheric pressure and room temperature, for example, at least 0 .5 mm H ₂ after reaction in 100 ml of water or at least 0.5 mm H ₂ after reaction in 500 ml of water.

In another aspect, the invention relates to a composition containing metallic magnesium, at least one acid and a binder, where the composition decomposes in less than 5 minutes, maintaining a pH of less than 7 10 minutes after decomposition and at least 0.5 mm H ₂ after contact with 50 ml of water in a container at atmospheric pressure and room temperature, for example, at least 0.5 mm H ₂ after reaction in 100 ml of water or at least 0.5 mm H ₂ after reaction in 500 ml of water.

In certain embodiments of any of the aspects described above, the composition passes a pharmaceutical friability test. In certain embodiments, the pH of the water is less than 7 10, 15, 20, 30, or 45 minutes after the composition has been exposed to water. In certain embodiments, the implementation of the pH of the water is less than 7 at least 1 hour after contact of the composition with water. In certain embodiments, the container is in communication with the atmosphere. In certain embodiments, the container is closed. In certain embodiments, when the container is closed, the pH remains at less than 7 7 days after contact with water. In certain embodiments, the magnesium in the composition reacts to form H ₂ as it breaks down in water, i.e. the decay rate and magnesium consumption rate are essentially the same.

The amount of magnesium metal is eg 5-500 mg, eg 5-100 mg. The amount of acid is eg 30-4000 mg, eg 200-400 mg. In certain embodiments, metallic magnesium and acid are present in amounts sufficient to maintain a pH of 4 to 6, and/or metallic magnesium and acid are present in amounts sufficient to achieve an H ₂ concentration of at least 2 mM in 50 ml of water in a container, for example, a closed or open container, for example, at least 2 mm H ₂ after reaction in 100 ml of water or at least 2 mm H ₂ after reaction in 500 ml of water. In certain embodiments, magnesium metal includes flakes, such as -325 caliber flakes. In other embodiments, magnesium metal is crushed to, for example, 200 gauge or less. In some embodiments, at least one acid is a food grade acid. The food acid is, for example, maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, tartaric acid, or a combination thereof. Exemplary food acids are tartaric acid and malic acid. In some embodiments, the acid is a cosmetically acceptable or pharmaceutically acceptable acid. Suitable for cosmetic purposes or pharmaceutically acceptable are, for example, acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentanepropionic acid, digluconic acid, dodecylsulfuric acid, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid, hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxy-ethanesulfonic acid, lactobionic acid, lactic acid, lauric acid, laurylsulfuric acid, malonic acid, methanesulfonic acid acid, 2-naphthalenesulfonic acid, nicotinic acid, nitric acid, oleic acid, palmitic acid, pamic acid, pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid a, propionic acid, stearic acid, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, or a combination thereof. Other acids include acetylsalicylic acid and 5-aminosalicylic acid. Examples of binders are mannitol, xylitol, maltose, dextrose and lactose. Illustrative binders are dextrose and lactose. In certain embodiments, when the acid is tartaric, citric, or ascorbic acid, the amount of magnesium is greater than 20 mg, such as at least 50 mg, or when the acid is acetylsalicylic acid and 5-aminosalicylic acid, the amount of magnesium is greater than 20 mg, for example at least 50 mg.

In addition, the composition may include a nutritional supplement, such as a magnesium salt, sweetener, flavor, color, flavor, essential oil, water-soluble lubricant, or polysaccharide. Exemplary polysaccharides include cellulose and its derivatives, such as methylcellulose or hydroxypropyl methylcellulose, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin. Illustrative lubricants include sodium stearyl fumarate and stearic acid, in particular sodium stearyl fumarate.

The invention also relates to a kit comprising the composition of the invention and a sealable container capable of holding 100 ml to 2 liters of water, eg 150-750 ml of water. In certain embodiments, the container has a double wall.

In addition, the invention relates to a method for producing hydrogen-rich water by bringing the composition of the invention into contact with water in a container, so that the composition breaks down and metallic magnesium and at least one acid react, for example, to form H ₂ in water at a concentration of at least least 0.5 mm H ₂ and the pH remains at less than 7 after 10 minutes after decomposition at atmospheric pressure and room temperature. In certain embodiments, the implementation of the water includes fruit juice, such as juice containing pectin. In other embodiments, the implementation of the concentration of H ₂ is at least 1 mm. In certain embodiments, a pH of less than 7 is maintained 1 hour after disintegration.

In addition, the invention relates to a method of administering hydrogen to an individual by providing the individual with a composition containing hydrogen produced from the composition of the invention, eg a tablet. In some embodiments, the hydrogen-containing composition is a nutraceutical or topical formulation. In one embodiment, the nutraceutical is a beverage.

In addition, the invention relates to compositions enriched with hydrogen, in which hydrogen gas is dissolved in the carrier at a concentration of at least 0.5 mm, for example, at a pH of less than 7. In some embodiments, the carrier is a food, cosmetic or pharmaceutical grade carrier. In some embodiments, the carrier is an aqueous liquid, cream, lotion, foam, paste, or gel. In some embodiments, the implementation of the composition is a drink. In certain embodiments, the maximum hydrogen concentration is 20 mM. In some embodiments, the composition has a pH of 4-6. In one embodiment, the pH is 4.6 or lower. In some embodiments, the implementation of the composition contains a nutritional supplement. In one embodiment, the nutritional supplement contains magnesium ions, potassium ions, or calcium ions. In some embodiments, the composition contains a sweetener, flavor, color, flavor, essential oil, or polysaccharide. In some embodiments, the composition contains a binder or a water-soluble lubricant.

In addition, the invention relates to compositions for producing acidic hydrogen enriched water. In one embodiment, the invention relates to a composition, such as a tablet, comprising magnesium metal, a food acid, and a binder. Typically, metallic magnesium and food acid are present in amounts sufficient to provide a pH of less than 7 and at least 0.5 mm H ₂ after reaction in 500 ml of water in a closed container. The invention also relates to a kit comprising this composition of the invention, eg a tablet, and a sealable container capable of containing 200 ml to 2 liters of water, eg 250-750 ml of water. In certain embodiments, the container is a double wall container. In addition, the invention relates to a process for producing hydrogen-enriched water by bringing this composition of the invention, for example, a tablet, into contact with water in a sealed container, so that the composition, for example, a tablet, disintegrates and metallic magnesium and acid react to form H ₂ in water at a concentration of at least 0.5 mm H ₂ and the pH is less than 7, for example, pH 4-6. In certain embodiments, the implementation of the water includes fruit juice, such as juice containing pectin. In other embodiments, the implementation of the concentration of H ₂ is at least 1 mm. The amount of metallic magnesium is, for example, 5-100 mg. In certain embodiments, magnesium metal and food acid are present in amounts sufficient to achieve a pH of 4 to 6, and/or magnesium metal and food acid are present in amounts sufficient to produce at least 2 mM H ₂ in 500 ml of water in a sealed container. container. In certain embodiments, magnesium metal is in powder form, such as 200 gauge or less. In other embodiments, magnesium metal includes flakes, such as -325 caliber flakes. The food acid is, for example, selected from the group consisting of maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid and oxalic acid. Examples of binders are mannitol, xylitol, maltose and lactose. In addition, the composition may include a vitamin, a mineral, such as a magnesium salt, a sweetener, a flavoring agent, a water-soluble lubricant, or a polysaccharide. Exemplary polysaccharides include methylcellulose, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.

Definitions

As used herein, the term "cosmetic" refers to a composition that is applied to all or part of the human body, such as the arms, face, shoulders, or legs, for cleaning, beauty, attractiveness, or appearance.

As used herein, the term "cosmetically acceptable" refers to a composition having ingredients that are acceptable for topical use in humans.

As used herein, the term "nutraceutical" refers to a composition having ingredients suitable for at least human consumption. Optionally, pharmaceutical grade ingredients may be used as described, for example, in "Remington: The Science and Practice of Pharmacy" (22nd ed.), ed. L.V. Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, PA.

As used herein, the term "passes the pharmaceutical friability test" refers to a composition that loses no more than 1% weight after 100 revolutions in a rotating drum friability tester such as from Copley Scientific.

As used herein, the term "pharmaceutically acceptable" refers to a composition having ingredients that meet U.S. pharmaceutical grade standards. Food and Drug Administration and, in addition, are controlled by the standards set in the U.S. Pharmacopoeia; this standard represents 99.9% purity of a particular ingredient.

As used in the context of the invention, the term "individual" refers to any animal that can be treated topically, orally, by inhalation or intravenously through a composition containing or used to produce H ₂ . Animals include fish, reptiles, birds (eg chicken, turkey) and mammals. Mammals that may be treated with compositions of the invention include primates (eg, humans, monkeys), livestock (eg, cows, pigs, sheep), draft animals (eg, bull, horse, llama) and companion animals (eg, dogs , cats).

DETAILED DESCRIPTION OF THE INVENTION

The present invention relates to the composition, for example, a tablet that breaks up in water with the formation of water enriched with hydrogen. Using the composition of the invention, for example in a ready-to-use container, supersaturated levels of H ₂ can be achieved that are significantly higher than the levels that can be achieved by adding pure gaseous H ₂ . In contrast to the previous compositions, the advantage of the present invention is the ability to obtain a hydrogen-rich composition that contains a supersaturated amount of H ₂ in an open container, i. at atmospheric pressure. In addition, the present invention relates to compositions that pass the pharmaceutical friability test, but still produce high levels of H ₂ . A further advantage of the invention is that the compositions can react rapidly, for example in less than 2 minutes, producing a consumable, for example potable, hydrogen rich product having H ₂ levels well above those of previous compositions.

The composition contains metallic magnesium, ie. elemental magnesium, an acid, and typically a binder and/or a lubricant. In water or a water-containing carrier, magnesium metal and acid react to form H ₂ , which is soluble in water, and magnesium ions. An advantage of the present invention is that the composition contains sufficient acid to maintain an acidic pH during H ₂ formation. When an insufficient amount of acid is used, the pH of the reaction mixture will increase, for example, until the solution becomes basic, which will cause the reaction to stop before high levels of H ₂ are reached. Without being bound by theory, at high pH, H ₂ production ceases due to the passivation of hydroxides and carbonates, which act as ligands for unreacted magnesium species. When this occurs, less magnesium metal is reacted, thereby reducing the amount of H ₂ produced available, leaving unacceptable levels of residual solids in the composition in the container. The use of an acid is also advantageous because a low pH, eg 4.6 or lower, helps to reduce microbial growth and thus reduce the likelihood of contamination. Thus, in certain embodiments, the invention relates to compositions that produce a hydrogen rich product having an acidic pH during use or storage.

metallic magnesium

Each composition contains a sufficient mass of magnesium to produce a sufficient volume of H ₂ in the volume of water to which it is added. Thus, in certain embodiments, the composition contains a sufficient mass of magnesium to form at least 0.1 mmol H ₂ , for example, at least 0.5 mmol, 1 mmol, 2 mmol, 3 mmol, 5 mmol or 10 mmol H _2, for example, at least 50, 75, 100, 125, 150, 175, 200, 225, 250, 500, 750, 1000, 1500 or 2000 ml of a suitable vehicle, for example water. Suitable masses of metallic magnesium include 5-1000 mg, e.g. or approximately 70 mg or 80 mg of magnesium.

The physical appearance, such as size and shape, of magnesium can be used to control the reaction rate. The particles may be spherical, spheroid, granular or flaky. Smaller particles and particles with higher surface area to volume ratios react with faster kinetics. You can also use mixtures of various sizes. Flaky magnesium has a higher surface area to volume ratio than granular magnesium. In certain embodiments, -325 caliber magnesium flake can be used in the compositions. Alternatively or additionally, larger magnesium or magnesium with a lower surface area to volume ratio may be used. For example, -200 caliber magnesium can be used. In other embodiments, +100, -100, +200, -200 (eg -200, +325), -325 or less magnesium is used. In certain embodiments, magnesium is provided in two sizes, eg -200 and -325, with the smaller size making up 20-50% of the total and the larger size making up the rest.

acids

Any water-soluble acid can be used within the scope of the present invention. The acid may be food grade, or otherwise cosmetic or pharmaceutical grade. Examples of food acids include, but are not limited to, maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, tartaric acid, and combinations thereof. Examples of cosmetic or pharmaceutical grade acids include acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentane propionic acid, digluconic acid, dodecylsulfuric acid, ethanesulfonic acid, glucoheptonic acid acid, glycerophosphoric acid, hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxyethanesulfonic acid, lactobionic acid, lactic acid, lauric acid, laurylsulfuric acid, malonic acid, methanesulfonic acid, 2-naphthalenesulfonic acid , nicotinic acid, nitric acid, oleic acid, palmitic acid, pamic acid, pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid, propionic acid, stearic acid, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of alpha acids (e.g. α-lupulic acid), polycarboxylic acids, Lewis acids, e.g. AlCl ₃ , and their combinations. Other acids include acetylsalicylic acid and 5-aminosalicylic acid. The acid is present in an amount necessary to react with the magnesium metal and optionally to maintain the pH below 7 when the composition is placed in water. It is preferred that the selected amount of acid is sufficient to maintain the pH at less than 6, eg 4 to 6, for the duration of the normal drinking time, eg at least 30 minutes or 1 hour. In certain embodiments, the number of moles of acid protons is at least 10%, 20%, 30%, 40%, 50%, 75%, or 100% greater than the number of moles of magnesium metal present. Suitable weight of acid includes 30-4000 mg, e.g. . An exemplary food acid is malic acid. Another exemplary food acid for use in the compositions of the invention is tartaric acid. Tartaric acid is highly water soluble with a water solubility of 0.125 g/mL. Acids with a solubility of about 0.01-1 g/ml, for example about 0.02-0.9 g/ml, about 0.03-0.8 g/ml, about 0.04 -0.7 g/ml, about 0.05-0.6 g/ml, about 0.06-0.5 g/ml, about 0.07-0.4 g/ml, about 0.08-0 .3 g/ml, about 0.09-0.2 g/ml, about 0.1-0.2 g/ml, about 0.11-0.5 g/ml, or about 0.12-0, 3 g/ml. When highly water-soluble acids are used in the composition of the invention, the composition is capable of rapidly disintegrating upon contact with water, for example allowing a more complete reaction with magnesium. This rapid dissolution has the advantage that the pH remains below 7 for a period of time corresponding to the consumption of the beverage, for example within 1-2 hours. Other such acids, both food grade and cosmetic and/or pharmaceutical grade, are known in the art.

The physical appearance, such as size and shape, of an acid can be used to control the rate of a reaction. For example, acids that are solid at room temperature, such as malic acid or tartaric acid, can be processed so that the particle size of the acid used to make the composition of the invention can be controlled. Smaller particles and particles with higher surface area to volume ratios react with faster kinetics. It is possible to use ground acid particles of various calibers, for example, from 40 caliber to 2500 caliber. Without wishing to be bound by theory, it is believed that the rate of dissolution of the composition depends linearly on the caliber. Compositions of the invention made with larger acid particles, such as 40-60 gauge, dissolve more slowly than compositions made with smaller acid particles, such as 120 gauge to 2500 gauge. Mixtures of acid particles of different sizes can also be used. Size controlled acid particles can be produced in a number of different ways, including, but not limited to, micronization, ball milling, or drum milling. Other methods for producing acid particles of controlled size are known in the art.

Binders

Any binder capable of disintegrating in water can be used. Examples of binders include sugars such as maltose, dextrose and lactose and sugar alcohols such as mannitol and xylitol. Exemplary binders for compositions of the invention include lactose and dextrose. Other binders for compositions are known in the art. The amount of binder is, for example, from 10 to 50% by weight of the composition, for example, 20-30%. Compositions of the invention may include a single binder, such as lactose, or they may be made from a combination of two or more binders to control the physical properties of the composition.

The binder may be a food grade, or otherwise cosmetic or pharmaceutical grade binder, as is known in the art, for example, from Remington (Remington: The Science and Practice of Pharmacy, (22nd ed.) ed. L.V. Allen, Jr. ., 2013, Pharmaceutical Press, Philadelphia, PA).

Additional components

The composition may also include other ingredients such as a food additive, sweetener, flavor, color, flavor, essential oil, lubricant, polysaccharide, or coating. The compositions of the invention may contain nutritional supplements such as vitamins, minerals and/or herbal extracts. For example, the composition may contain a magnesium, potassium or calcium salt. Suitable sweeteners are known in the art, for example, sucrose, mannose, sucralose, aspartame, saccharin, stevia, arhut extract, and acesulfame K. The composition may also include any food grade color, such as FD&C colors, and/or flavor, such as fruit flavored supplement. In addition, the composition may include an essential oil such as grape seed oil, wintergreen oil, lavender oil. Other essential oils are known in the art. In addition, the composition may include a fragrance, such as eucalyptus. The composition may also contain a polysaccharide such as psyllium fiber, cellulose and its derivatives such as methylcellulose or hydroxypropyl methylcellulose, various starches, apple powder, lemon powder, lime powder or grapefruit powder. Polysaccharides can increase the amount of H ₂ remaining after the reaction. In addition, the composition may include a water-soluble lubricant, such as micronized sodium stearyl fumarate or finely divided stearic acid, for example, having a size of 5 micrometers. Also, the composition may have a water-permeable coating, such as a soluble surfactant, to control the rate at which the composition dissolves. The soluble surfactant coating can be a triblock copolymer, eg a poloxamer, eg poloxamer 407, or a pharmaceutically acceptable non-ionic polymeric surfactant, eg glucosides. For example, the composition may have a coating that dissolves in less than 5 minutes, such as less than 1 minute, allowing the consumer to close the container before the composition begins to disintegrate and H ₂ production begins.

Previous attempts to prepare effervescent compositions, e.g. tablets, using typical lubricants such as sodium lauryl sulfate as described in US Patent Publication 2016/0113865 and sodium stearyl fumarate have not been successful in producing tablets that disintegrate rapidly. This was a consequence of the use of a higher amount of lubricant required for tablet formation. The use of large amounts of non-micronized lubricant resulted in a tablet with a long disintegration time, which further led to an excess of undissolved residues in the container and an unpleasant taste. In contrast, significantly less lubricant can be used in the compositions of the invention, resulting in faster reaction kinetics, a satisfactory amount of residue, and a pleasant taste.

Forms of composition

The composition can be composed in the form of a tablet. The tablet may be in any suitable form. For example, a tablet may be a disc, a sphere, or an ovoid. One tablet usually contains the amount of magnesium and acid required to form the required amount of H ₂ in a given volume of water, for example 50, 150 or 500 ml. However, a combination of several smaller tablets can be used. For example, the tablets may be sized to provide sufficient H ₂ in 250 ml, and multiple tablets may be used for larger volumes. Because the reaction of magnesium metal and acid is activated by water, compositions of the invention are typically stored in waterproof packaging such as foil or plastic. The tablet components are also usually non-hygroscopic, however, hygroscopic ingredients can be used if the tablet is packaged in a dry, waterproof container or wrapper. Tablets can be made by methods known in the art.

A factor to consider when forming the compositions of the invention into tablets are the physical properties of the tablet, eg friability. Friability is defined as the tendency of a tablet to crack, crumble, or break after compression or other processing. Tablet friability is evaluated using a rotating drum and measuring the percentage weight reduction of the tablet after rotation in the drum for a fixed number of drum revolutions. For a tablet to pass the friability test, the weight of the tablet must only decrease by no more than 1% after 100 revolutions in the rotating drum. For the compositions of the invention, friability is controlled by the type and size of the acid grains used in the composition, the type and size of the binder grains, the type and size of the lubricant grains, and the pressure at which the tablets are compressed in the mold. The use of finer particles generally results in tablets with greater friability. As a result, tablets made from finely divided particles are often made under high pressure to ensure that they do not collapse; this results in a tablet that is very hard, reducing the rate at which it can disintegrate on contact with water. Thus, small caliber acid tablets can be prepared from a highly water soluble acid such as tartaric acid to support the hydrogen generation reaction.

Other forms of composition may also be used. For example, the composition may be provided in the form of a powder, for example, inside a water-soluble capsule or a water-permeable bag, or small or large granules, such as bath bombs, or a film.

The dissolution time of the composition, and thus the measured H ₂ concentration, is controlled by the percentage by weight of the binder, the percentage by weight and type of lubricant, the ratio of acid to magnesium, the physical properties of both magnesium and acid, for example, caliber and physical conditions in which composition is located. Compositions of the invention typically disintegrate upon contact with water in the container in less than 5 minutes, eg less than 4 minutes, less than 3 minutes, less than 2 minutes, or less than 1 minute.

The temperature of the water in which the composition is located affects how quickly the composition breaks down. Hot water will rapidly decompose the composition, but will not retain a high concentration of hydrogen gas. Colder water increases the solubility of hydrogen in water, but does not ensure rapid decomposition of the composition. A suitable temperature for the formation of hydrogen from the composition according to the invention is approximately room temperature, for example, 15°C -25°C, for example, 15°C, 16°C, 17°C, 18°C, 19°C, 20°C, 21°C, 22°C, 23°C, 24°C, or 25°C, such as 59°F-77°F, such as 59°F, 60°F. 61°F, 62°F, 63°F, 64°F, 65°F, 66°F, 67°F, 68°F, 69°F, 70°F, 71°F, 72°F, 73° F, 74°F, 75°F, 76°F or 77°F.

The compositions will maintain a hydrogen rich acid product, eg having a pH less than 7, eg 4-6, for at least some period of time after contact with water. The acidic pH can be maintained for a typical period of time for the application of a hydrogen enriched product, such as 10 minutes after contact of the composition with water. For example, the composition of the invention maintains a pH less than 7 for at least 5 minutes, for example, 5-300 minutes, 10-250 minutes, 15-200 minutes, 20-150 minutes, 25-120 minutes, 30-100 minutes, -90 minutes, e.g. at least 5 minutes, at least 10 minutes, at least 15 minutes, at least 20 minutes, at least 25 minutes, at least 30 minutes, at least 35 minutes, at least at least 40 minutes, at least 45 minutes, at least 50 minutes, at least 55 minutes, at least 60 minutes, at least 70 minutes, at least 80 minutes, at least 90 minutes, at least 100 minutes, at least 110 minutes, at least 120 minutes, at least 130 minutes, at least 140 minutes, at least 150 minutes, at least 160 minutes, at least 170 minutes, at least 180 minutes, at least 190 minutes, at least 200 minutes, at least 250 minutes, or at least 300 minutes, such as at least 0.5 hours, at least at least 1 hour, at least 1.5 hours, at least 2 hours, at least 2.5 hours, at least 3 hours, at least 3.5 hours, at least 4 hours, at least 4.5 hours, or at least 5 hours. The compositions can also maintain a pH of less than 7 for an extended period of time, such as one day, seven days, 30 days, or 6 months after the composition has been exposed to water. Moreover, the pH of the hydrogen-enriched product can then become alkaline, for example, more than 7.

For compositions intended for use as a cosmetic shower or bath additive, the dissolution rate of the tablet is an important factor. The composition must dissolve slowly enough in water to provide a constant level of H ₂ during the time spent in the shower or bath. An additional limitation is the thermodynamics of the dissolution reaction since the reaction is exothermic and produces small amounts of magnesium hydroxide. If the reaction is too fast, the end temperature of the bath may become too high or too much magnesium hydroxide may be produced; both of these effects can damage the skin. The addition of polysaccharides to the compositions has been shown to have an effect on dissolution rate while maximizing retained H ₂ . The added polysaccharide may be a fibrous polysaccharide such as cellulose and its derivatives, for example hydroxypropyl methylcellulose (HPMC, known as hypromellose). Alternatively or additionally, the addition of a soluble surfactant such as a triblock copolymer (eg, poloxamer 407) can be used to delay tablet dissolution, ensuring sufficient magnesium consumption and maximizing the time period that H ₂ is dissolved in water.

Hydrogen enriched liquids for use as a cosmetic or beauty spray may have a higher acid content and the resulting composition may utilize the skin's natural pH of 4.5-5.2 (Lambers et al., Int. J. Cosmet Sci. , 2006, 28, 359-370) to further increase the H ₂ concentration. It was shown that H ₂ provides many benefits for the skin and the use of a cosmetic spray as a cleansing agent to return the skin of its natural significance PH can provide additional health benefits.

carriers

Compositions of the invention, for example tablets, are administered by bringing them into contact with a carrier such as water or other aqueous liquid. The water may be pure, such as deionized, or may contain other dissolved ions, such as in spring or tap water. The water may also contain other ingredients, for example, it may be or may contain fruit juice, or may contain other dissolved gases, such as in carbonated water, or dissolved solids, such as table sugar or salt. An exemplary fruit juice is lemon juice.

The carrier volume is chosen based on the use of enriched hydrogen. When the composition of the invention is used to prepare a beverage, the volume of liquid, such as water or fruit juice, to be enriched is from about 100 ml to 2 liters, for example, about 100 ml, about 150 ml, about 200 ml, about 250 ml, about 300 ml, approximately 350 ml, approximately 400 ml, approximately 450 ml, approximately 500 ml, approximately 550 ml, approximately 600 ml, approximately 650 ml, approximately 700 ml, approximately 750 ml, approximately 800 ml, approximately 850 ml, approximately 900 ml, approximately 950 ml, approximately 1 liter, approximately 1.5 liters or approximately 2 liters. When the composition of the invention is used to prepare a cosmetic product, the amount of water is about 50 ml to 500 ml, for example, about 50 ml, about 100 ml, about 150 ml, about 200 ml, about 250 ml, about 300 ml, about 350 ml , approximately 400 ml, approximately 450 ml or approximately 500 ml.

Alternatively, water may be present in a topical vehicle such as a cream, lotion, foam, paste or gel so that the H ₂ can be effectively delivered to the skin. Methods for making water-soluble topical carriers are well known in the art, for example, as described in Remington (Remington: The Science and Practice of Pharmacy, (22nd ed.) ed. LV Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, PA ) and in the cosmetics industry. During or after the reaction of the composition of the invention with water, the carrier may be mixed, agitated or shaken to provide a uniform consistency.

Containers

Various containers can be used to bring the composition into contact with a body of water. In one embodiment, the container has a lid that can be used to close the container, for example shortly after adding the composition to a bulk of water. The closed container retains the formed H ₂ while the reaction comes to completion. Alternatively, H ₂ may be produced in an open container. An example of a suitable container is a double walled stainless steel bottle with a double liner.

APPLICATIONS

Compositions of the invention, for example tablets, are used by bringing them into contact with a carrier which promotes dissolution of the composition. An illustrative carrier is water. Typically, the amount of water used to dissolve the composition is from 50 ml to 2 liters, for example 50 ml, 150 ml, 250 ml, 355 ml, 500 ml, 750 ml or 1 liter. The user may add the composition to water or other vehicle in a sealed container and allow the reaction to proceed for 1 or more minutes depending on the temperature of the water, for example 1-2 minutes, at least 5 minutes, 10 minutes, 15 minutes, 30 minutes, 45 minutes, 60 minutes, 90 minutes, or 12 hours. In certain embodiments, it is preferred that the composition react in less than 2 minutes. Preferably, the tablet and volume of water provide a concentration of at least 0.5 mM, such as at least 1 mM, at least 3 mM, at least 5 mM, or at least 10 mM, such as 0.5-20 mM, 1-15 mM or 5-10 mM. The inclusion of polysaccharide, either in the composition, or in water or media, for example, in fruit juice, can increase the concentration of H ₂ relative to the reaction in the absence of polysaccharide, or locally near polysaccharide, or in enriched H ₂ composition as a whole.

Drinking hydrogen-enriched water is known in the art to help treat various disorders including Parkinson's disease (Yoritaka et al., BMC Neurology, 2016, 16:66), depression (Zhang et al. Sci. Rep . 2016; 6:23742) , periodontitis (Azuma et al. Antioxidants (Basel) . 2015; 4(3):513-22), type II diabetes, metabolic syndrome, chronic renal failure, inflammation, rheumatoid arthritis, interstitial cystitis, cerebral ischemia, hyperlipidemia, chronic hepatitis B and others, as described in Ichihara et al. ( Med. Gas Res . (2015) 5:12). Thus, the compositions of the present invention may be used by individuals suffering from any of these disorders to treat the disorder or alleviate one or more of its symptoms.

In addition, H ₂ has been shown to be effective in the treatment of various dermatological conditions. For example, when the composition of the invention is used to prepare a hydrogen-enriched aqueous liquid, the pH of the resulting aqueous liquid can be adjusted to produce "beauty water" with a pH of 4.5-5.5, which has a variety of health benefits (Lambers et al., Int. J. Cosmet. Sci. 2006, 28, 359-370). "Beauty water" has been used as a base carrier for topical magnesium ion cosmetics, with the lower pH and _H2 content effectively promoting magnesium absorption through the skin ( Magnes. Res. 2016; 29(2):35-42 ). It was shown that in another example, the products containing H ₂ are promising for the treatment of local skin conditions, such as wrinkles, atopic dermatitis and UV-induced skin burns ( Mol. Cell. Toxicol. 2013, 9 (1), 15-21). For local testimony, the composition of the invention can be directly included in a dermatological medium, such as cream, lotion, foam, pasta or gel.

Hydrogen-containing products obtained from the production of H ₂ in situ can be used to improve the health of certain farm animals, in particular dairy cows. I believe that H ₂ can potentially increase the duration of use and life of dairy cows, which leads to an increase in milk production.

The compositions of the invention can also be used to provide inhalable hydrogen gas, for example by inhaling the gas as it is released, either from an open container or through a cannula or nasal tube.

HYDROGEN ENRICHED ACID COMPOSITIONS

The composition of the invention can be used to manufacture a range of products, including but not limited to food and nutraceuticals (e.g. drinks), and skin care products, such as lotions, bath bombs, or shower tablets, for effective delivery of H ₂ On the skin. In certain embodiments, the hydrogen enriched composition is a beverage in an open container. In the case of local compositions, the composition of the invention can be directly included in the local carrier of the pharmaceutical category or cosmetic category, such as cream, lotion, foam, pasta or gel. Compositions for topical application containing H ₂ can be impregnated into the skin, they can be applied with a roller, rubbed or applied directly to the skin.

For products intended for human ingestion, such as nutraceuticals, such as beverages, the acid used to prepare the composition of the invention must be safe for consumption, as in the case of food acids described in this description (for example, malic acid or tartaric acid) . The acid used in the composition of the invention for the manufacture of topical products may be any pharmaceutically or cosmetically acceptable acid and its counterion that is "generally considered safe" as defined by the US Food and Drug Administration for use in humans and in veterinary medicine. Representative acids include acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentane propionic acid, digluconic acid, dodecylsulfuric acid, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid. , hemisulfuric acid, heptonic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxyethanesulfonic acid, lactobionic acid, lactic acid, lauric acid, lauryl sulfuric acid, malonic acid, methanesulfonic acid, 2-naphthalenesulfonic acid, nicotinic acid, nitric acid, oleic acid, palmitic acid, pamoic acid, pectic acid, persulfuric acid, 3-phenylpropionic acid, phosphoric acid, picric acid, pivalic acid, propionic acid, stearic acid, chamois th acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of alpha acids (eg α-lupulic acid), polycarboxylic acids, Lewis acids, eg AlCl ₃ , and combinations thereof. Other such acids are known in the art.

The hydrogen-rich water produced from the composition of the invention has a dissolved H ₂ concentration of 0.5 mM to 20 mM, for example 1 mM to 15 mM, 1 to 10 mM, 1 mM to 4 mM, 1 mM to 3 mM, 1 mM to 2 mM, 1.5 mM to 4 mM, or 2 mM to 3 mM, e.g., about 0.5 mM, about 1 mM, about 1.5 mM, about 2 mM, about 3 mM, about 4 mM, about 5 mM, about 6 mM, about 7 mM, about 8 mM, about 9 mM, about 10 mM, about 15 mM, or about 20 mM. In other embodiments, the implementation of the concentration is from 1 ppm. up to 3 ppm, from 2 ppm up to 4 ppm, from 3 ppm up to 6 ppm, from 4 ppm up to 8 ppm, from 5 ppm up to 10 ppm, from 6 ppm Up to 12 M.D. or from 5.D. up to 15 m.d.

The acid content of the composition used to enrich the water with hydrogen may be sufficient to maintain the pH at less than 7, eg less than 6, eg 4-6, while consuming a sufficient amount of magnesium. The hydrogen-enriched composition may also include a food additive, such as a magnesium salt, a sweetener, a flavoring agent, a coloring agent, a fragrance, an essential oil, a water-soluble lubricant, or a polysaccharide.

EXAMPLES

Example 1

In this example, hydrogen enriched water was prepared by dissolving the following two compositions in separate open containers and monitoring the concentration of hydrogen released over time.

Sample composition #1-"F6" - dissolved in 500 ml of water having a temperature of 17°C

80 mg Magnesium -325 Caliber Flakes

120 mg tartaric acid, caliber 120

200 mg malic acid, caliber 120

200 mg dextrose

6 mg sodium stearyl fumarate

Composition sample #2 - "F1" - dissolved in 500 ml of water having a temperature of 17°C

55 mg magnesium, caliber -200, ground

25 mg magnesium, caliber -325, flake

340 mg malic acid, caliber 60

160 mg lactose

6 mg sodium stearyl fumarate

Composition F6 containing 120 gauge fine acid particles dissolved faster (about 1.75 minutes) than composition F1 with larger 60 gauge grit particles (about 3.5 minutes). If the acids were only ground to 60 gauge in formulation F6, the tablet dissolution time was approximately 3 minutes. Both Composition F6 and Composition F1 passed the minimum pharmaceutical friability test. The following experimental data, using ground tartaric acid particles of less than 10 micrometers in the F6 formulation instead of 120 gauge particles, demonstrated a tablet dissolution time of 45 seconds. In addition, by using dextrose instead of lactose as the binder, the dissolution time per tablet was reduced by approximately 30 seconds while still allowing the friability to remain within acceptable limits.

The hydrogen concentration reached by composition F6 after it had completely decomposed was 9 ppm. For composition F1, the hydrogen concentration after complete decomposition was 3.5 ppm. A similar composition that failed the friability test produced a maximum hydrogen concentration of 12 ppm. approximately 75 seconds later. All concentration data were the average of approximately 20 individual tablets of each formulation.

In a second experiment, the dissolution of a composition containing both tartaric acid and malic acid ("F35") was examined with the following ingredients:

60 mg Magnesium -325 Caliber Flakes

90 mg tartaric acid

150 mg malic acid

150 mg dextrose

6 mg sodium stearyl fumarate

Under identical aqueous conditions with F1 and F6 (eg 500 ml of water in an open container at 17°C), the concentration was 5.3 ppm. after a reaction time of approximately 80-90 s. The concentration measured was the average of approximately 20 tablets.

Example 2

An exemplary tablet for use in preparing a hydrogenated ready-to-drink beverage includes the following components:

30 mg Magnesium caliber -200

30 mg magnesium -325 flake

90 mg tartaric acid

150 mg malic acid

150 mg dextrose

5.5 mg 2500 caliber stearic acid

Example 3

A tablet for use in making a hydrogenated beverage in a closed container contains the following ingredients:

55 mg magnesium -200 caliber

25 mg magnesium -325 flake

310 mg malic acid

100 mg magnesium malate

160 mg lactose

7 mg sodium stearyl fumarate

These ingredients were compressed into a tablet using a manually operated mechanical tablet press. This tablet, when dissolved in water in a 500 ml airtight container, forms H ₂ gas. In a standard soda bottle (500 ml), the concentration of H ₂ reached 1.6 ppm. (0.8 mm) within 15 minutes, 4 pm (2 mm) within 2 hours and exceeded 6.D. (3 mM) within 12 hours. In a stainless steel bottle with a double wall and a double seal, the concentration reached 2.8 ppm. (1.4 mM) after 15 minutes, 3.8 ppm (1.9 mm) after 1 hour and exceeded 7 ppm. (3.5 mm) after 12 hours. The pH of the final solution when the tablet was added to plain water was 4-6.

When fruit juice, including fruit juices with a high pectin content such as lemon, lime, apple and orange juice, is used as a liquid or in addition to a liquid, the concentration of H ₂ in the foam above the liquid may exceed 20 ppm. (10 mm). An increase in the concentration of H ₂ was also observed in the case of pre -added pectin (Certo®) and the husks of plantain seeds.

Example 4

A tablet intended for use in a beverage to produce a high concentration of H ₂ includes the following components:

30 mg magnesium

200 mg malic acid

Sufficient amounts of both binder and lubricant

These ingredients can be compressed into a suitably shaped tablet in a 9-11 mm diameter tablet die.

Example 5

A tablet intended for use as a cosmetic product, shower product or bath product, contains the following components:

480 mg magnesium

720 mg tartaric acid

1200 mg of apple acid

Sufficient amounts of both binder and lubricant to bring the tablet weight up to 3600 mg.

These ingredients can be compressed into a suitably shaped tablet in a 24 mm diameter tablet die.

Example 6

The second tablet intended for use as a cosmetic product, whether the shower means for a bath, includes the following components:

240 mg Magnesium caliber -325

360 mg 80 gauge tartaric acid (or lower)

600 mg 80 gauge malic acid (or lower)

Sufficient amounts of both binder and lubricant to bring the tablet weight up to 1800 mg.

These ingredients can be compressed into a suitably shaped tablet in an 18 mm diameter tablet press.

Example 7

A tablet intended for use in a beverage or cosmetic spray contains the following ingredients:

80 mg of magnesium caliber -325

120 mg 80 gauge tartaric acid (or lower)

200 mg 80 gauge malic acid (or lower)

Sufficient amounts of both binder and lubricant to bring the tablet weight to 600 mg.

These ingredients can be compressed into a suitably shaped tablet in a 12 mm diameter tablet press.

Example 8

A tablet intended for use in a beverage or cosmetic spray contains the following ingredients:

60 mg magnesium

90 mg tartaric acid

200 mg of apple acid

Sufficient amounts of both binder and lubricant to bring the tablet weight up to 4500 mg.

These ingredients can be compressed into a suitably shaped tablet in a 12 mm diameter tablet press.

Example 9

A tablet designed for use exclusively in a cosmetic spray or spray for beauty includes the following components:

25-40 mg magnesium

A sufficient amount of acid in excess of the amount in the tablets used to obtain an enriched drink.

Sufficient amounts of both binder and lubricant.

These ingredients can be compressed into a suitably shaped tablet in a 9 mm diameter tablet press.

Example 10

The advantage of a tablet containing magnesium particles in the form of small flakes is that the H ₂ molecules are released sequentially. When sufficient acid is present and the mass of magnesium in the tablets corresponds to the volume of liquid to be saturated with H ₂ (at least 80 mg of magnesium and 300 mg of acid in total per 500 ml of liquid), H ₂ will continuously be released, first creating bubbles of H ₂ the size of picometer range, which then merge into nanometer-sized bubbles, then micrometer-sized bubbles, and then into larger bubbles. Nano-sized bubbles are able to saturate an aqueous solution to a greater extent than bubbles of other sizes, and thus they can create a higher H ₂ pressure in the liquid. This is a result of larger bubbles coming out of solution, but nanometer-sized bubbles are more stable, and the physicochemical properties of nanometer-sized bubbles differ from those of individually dissolved H ₂ molecules, which change according to Henry's Law and the gas fugacity coefficient. Increased pressure stops the reaction according to Lechatelier's principle, leaving sub-micron sized magnesium flakes in solution. As the H ₂ bubbles merge and further dissipate, the pressure in the system drops and an equivalent amount of magnesium magnesium reacts, further producing H ₂ .

This continuous reaction allows the concentration of H ₂ formed to exceed 3 ppm when the composition is placed in an open container rather than a closed bottle, for example, at a pressure of 1 atmosphere, but allows continuous replenishment of H ₂ to bring the local H ₂ concentration to approximately up to 9 M.D. The rate of disintegration of the tablet and the subsequent reaction of magnesium and acid can be increased by selecting tablet components, e.g., coatings or binders, to control the reaction kinetics, with the reaction reaching completion in no more than 4 minutes, e.g., in the range of 1-2 minutes.

The use of cold water to dissolve the compositions of the invention allows an increased concentration of hydrogen to be maintained, but also causes a significant slowdown in the dissolution of the tablet and, as a result, in the overall hydrogen formation reaction. For example, in water at a temperature near freezing (1° C.), the tablets of the invention typically take 4-5 minutes to completely dissolve. Although, when the water is saturated, the dissolved hydrogen is retained for a longer period of time in the water at a higher concentration. The use of hot water to dissolve the composition of the invention leads to a significant increase in the rate of dissolution and, therefore, to a faster release of hydrogen. For example, in hot water, for example, at a temperature above room temperature, the invention tablets usually completely dissolve for 1 minute or less. However, the merger rate increases significantly with an increase in temperature, thus reducing the retention time and the total stability of enriched water.

Using current technology and tabletting capabilities, the ideal water temperature range for dissolving a tablet made from the composition of the invention is 12-20°C, depending on the final tablet formulation.

Example 11

The composition of the invention, eg a tablet, is capable of dissolving and providing a semi-stable supersaturation of H ₂ in an open container, eg at room temperature. Polysaccharides contained in the composition or present in a liquid medium are able to form a border layer on the surface of the liquid. This boundary layer prevents the rapid dissipation of the H ₂ gas cloud that forms when the composition dissolves. For example, in a rigid container, the addition of a pH modifier, such as 2 teaspoons of lemon juice (which contains pectin) or vinegar, increases the available H ₂ concentration. The use of vinegar results in a higher concentration of H ₂ in the liquid. When water and lemon juice are placed in a standard soda bottle made primarily of polyethylene terephthalate (PET), the _H2 concentration rises 6-7 times at the top of the gas cloud. In an open glass bottle with the same solution of water and lemon juice, the concentration of H ₂ gas produced increases by approximately 20%. When polysaccharides are used, foam is formed on the surface of the liquid, which includes a higher concentration of H ₂ relative to the rest of the liquid.

Open containers are able to quickly create a suspension of magnesium nanoparticles after the tablet is placed in the container. This increases the rate of reaction of the formation of H ₂ . For example, in a tablet that fully reacts within 30 to 60 seconds, the bubbles formed on the surface burst vigorously and result in a measured H ₂ concentration of 1.6 ppm.

For the composition of the invention, the ideal reaction rate is 70-90 seconds, often reaching supersaturation in the gas cloud of 10 ppm. The measured H ₂ concentration appears to decrease linearly over time, as shown in the data presented in Table 1, reaching a typical SATP concentration of 1.6 ppm. After dissolving for 8 minutes.

Table 1. Measured concentration of H ₂ after dissolution of the composition according to the invention

Dissolving time (c) Measured concentration h ₂ (ppm) 80-90 10 150 6 180 4.5-5 210 3.5-4 300 2.2-2.5 360 1.8 480 1.6

Example 12

In this example, H ₂ enriched water obtained by dissolving a composition of the invention, eg a tablet, in an open container was transferred to a resealable glass bottle with a screw cap and allowed to stabilize under pressure as the composition was further dissolved. When the closed bottle was opened, the measured concentration H ₂ was 5.3 p.

In the following experiment, H ₂ enriched water, obtained by dissolving a composition of the invention, eg a tablet, in an open container was transferred to a resealable PET soda bottle modified to include a pressure gauge to detect the pressure inside the bottle. As the reaction passes, the pressure in the bottle began to increase, creating free space in the bottle as it was formed with the subsequent dispersion of bubbles H ₂ . After reacting for 5 minutes, the bottle pressure measured was 25 psi. Inch (172.4 kPa) and after the reaction for 30 minutes the measured pressure in the bottle was 45 pounds/sq. inch (310.3 kPa). At this pressure, the measured concentration of H ₂ was 2.3 ppm.

The composition in both containers (open and closed bottle) continued to react with micrometer-sized particles. As the H ₂ coalesced and dissipated, the pressure contained within the liquid was transferred to the free space, increasing the pressure in the container. Remarkably, the pressure achieved by transferring the liquid from the open container into the PET bottle reaches and even exceeds the pressure created by dropping the tablet into the PET bottle and sealing immediately thereafter. The same tablet provides approximately 35 psi. Inch (241.3 kPa), when the closure was carried out immediately, due to the stop of the reaction according to the principle of the Leshtel, thus also confirming the ability of the composition to oversaturation.

Example 13

One of the variables that controls the generation of hydrogen from the composition of the invention is the mass of magnesium used to react with the milled acid. The relationship between the mass of magnesium and the concentration of dissolved hydrogen is approximately linear - as the amount of magnesium used increases, the amount of hydrogen produced at a fixed mass of acid increases. Table 2 presents hydrogen concentration data for various masses of magnesium, where the acid was ground to a fine particle size (~120 caliber), and a dissolution time of approximately 60-75 s.

Table 2. Measured concentrations H ₂ after dissolving the composition of the invention made of caliber acid ~ 120

Mass of magnesium (mg) Measured concentration H ₂ (ppm) 80 9-12 70 N/A 60 4-5 55 3 50 2.6-3

The effect of grinding acids was also investigated by performing size distribution determinations by laser diffraction on the bubbles produced during the dissolution reaction. When finely divided acids were used, the resulting bubbles exhibited a bimodal distribution with the first mode corresponding to a diameter of approximately 50-60 nm and the second mode corresponding to a diameter of 600 nm after noise correction. As noted in Example 10, nanometer-sized bubbles are able to saturate an aqueous solution to a greater extent than bubbles of other sizes, and thus can create a higher H ₂ pressure in the liquid, thus confirming the importance of using finely divided acids in the production of compositions for water enrichment with hydrogen.

Additional open container testing using a tablet made from finely divided acid demonstrated the formation of 70 ml of hydrogen gas at a theoretical limit of 80 ml during the first 80-90 seconds. By the second minute of the reaction, only 6 ml of hydrogen gas had escaped from the surface of the liquid in the open container.

Claims (118)

1. Composition for obtaining hydrogen-enriched water, containing: 60-100 mg of metallic magnesium; at least one food acid; And a binder, where the binder is a sugar; Where the composition is a tablet, which breaks up for less than 5 minutes when contacting water and reacts with the formation of 3-20 mm of the dissolved and suspended H ₂ in an open container, when it breaks up into 500 ml of water. 2. The composition of claim 1, wherein the composition passes a pharmaceutical friability test. 3. The composition of claim 1, wherein the composition disintegrates in less than 2 minutes. 4. The composition of claim 1, wherein the pH of the water remains less than 7 for at least 10 minutes after the composition has been contacted with water. 5. The composition of claim 1 wherein the magnesium metal comprises flakes. 6. The composition of claim 1 wherein the magnesium metal comprises -325 gauge flakes. 7. The composition of claim 1 wherein the magnesium metal is particulate. 8. The composition of claim 1 wherein the magnesium metal is 200 gauge or less. 9. The composition of claim 1 wherein at least one food acid is selected from the group consisting of maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid and tartaric acid, or their mixtures. 10. The composition of claim 1, wherein the at least one food acid is tartaric acid. 11. The composition of claim 1, wherein at least one food acid is malic acid. 12. The composition of claim 1 wherein the at least one food acid is 60 gauge or less. 13. The composition according to claim 1, where the amount of at least one food acid is 30-4000 mg. 14. Composition according to claim 1, where the binder is maltose, dextrose or lactose. 15. The composition of claim 1 further comprising a water-soluble lubricant. 16. The composition of claim 1 wherein the water-soluble lubricant is selected from sodium stearyl fumarate or stearic acid. 17. The composition of claim 1 wherein the water-soluble lubricant is sodium stearyl fumarate. 18. The composition of claim 1, wherein the composition maintains a pH of less than 7 7 days after contact with water. 19. The composition according to claim 1, additionally containing a nutritional supplement. 20. The composition of claim 19, wherein the food additive is a magnesium salt. 21. The composition according to claim 1, additionally containing a sweetener or flavoring agent. 22. The composition according to claim 1, additionally containing a dye. 23. The composition according to claim 1, additionally containing a perfume. 24. Composition for obtaining hydrogen-enriched water, containing: 60-100 mg of metallic magnesium; at least one water-soluble food acid; And a binder, where the binder is a sugar; where the composition reacts to form H ₂ because it decomposes on contact with water, where the composition is a tablet, and where the composition produces from 3-20 mm dissolved and suspended H ₂ in an open container when it disintegrates in 500 ml of water and where at least one water-soluble food acid has a solubility of at least 0.01 g/ml. 25. The composition of claim 24, wherein the composition passes a pharmaceutical friability test. 26. The composition of claim 24, wherein the composition disintegrates in less than 2 minutes. 27. The composition of claim 24 wherein the magnesium metal comprises flakes. 28. The composition of claim 24 wherein the magnesium metal comprises -325 gauge flakes. 29. The composition of claim 24 wherein the magnesium metal is particulate. 30. The composition of claim 24 wherein the magnesium metal is 200 gauge or less. 31. The composition of claim 24, wherein the at least one water-soluble food acid has a water solubility of at least 0.05 g/mL. 32. The composition of claim 24, wherein the at least one water-soluble food acid has a water solubility of at least 0.1 g/mL. 33. The composition of claim 24, wherein the at least one water-soluble food acid has a water solubility of at least 1 g/mL. 34. The composition of claim 24, wherein the at least one water-soluble food acid is selected from the group consisting of maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, and tartaric acid. , or mixtures thereof. 35. The composition of claim 24, wherein the at least one water-soluble food grade acid is tartaric acid. 36. The composition of claim 24, wherein the at least one water-soluble food acid is malic acid. 37. The composition of claim 24, wherein the at least one water-soluble food acid is 60 gauge or less. 38. The composition according to claim 24, wherein the amount of at least one water-soluble edible acid is 30-4000 mg. 39. The composition of claim 24 wherein the binder is maltose, dextrose or lactose. 40. The composition of claim 24 wherein the binder is dextrose. 41. The composition of claim 24, wherein the binder is lactose. 42. The composition of claim 24, further comprising a water-soluble lubricant. 43. The composition of claim 24, wherein the water-soluble lubricant is selected from sodium stearyl fumarate or stearic acid. 44. The composition of claim 24 wherein the water-soluble lubricant is sodium stearyl fumarate. 45. The composition of claim 24, wherein the composition retains a pH of less than 7 7 days after contact with water. 46. The composition according to claim 24, additionally containing a nutritional supplement. 47. The composition of claim 46 wherein the nutritional supplement is a magnesium salt. 48. The composition according to claim 24, additionally containing a sweetener or flavoring agent. 49. The composition according to claim 24, additionally containing a dye. 50. Composition for obtaining hydrogen-enriched water, containing: 600-100 mg of metallic magnesium; at least one food acid; And binder, where the binder is a sugar, where the composition reacts to form H ₂ as it decomposes on contact with water, where the composition is a tablet, and where the composition produces from 3-20 mM dissolved and suspended H ₂ in an open container when it decomposes in 500 ml of water and maintains pH less than 7 10 minutes after contact. 51. The composition of claim 50, wherein the composition passes a pharmaceutical friability test. 52. The composition of claim 50, wherein the pH is less than 7 after 30 minutes of contact with water. 53. The composition of claim 50 wherein the pH is less than 7 approximately 1 hour after contact with water. 54. The composition of claim 50 wherein the magnesium metal comprises flakes. 55. The composition of claim 50 wherein the magnesium metal comprises -325 caliber flakes. 56. The composition of claim 50 wherein the magnesium metal is particulate. 57. The composition of claim 50 wherein the magnesium metal is 200 gauge or less. 58. The composition of claim 50 wherein the food acid is selected from the group consisting of maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid and tartaric acid, or mixtures thereof. 59. The composition of claim 50 wherein at least one acid is tartaric acid. 60. The composition of claim 50 wherein at least one acid is malic acid. 61. The composition of claim 50 wherein at least one acid is 60 gauge or less. 62. The composition according to p. 50, where the binder is a maltose, dextrose or lactose. 63. The composition of claim 50, further comprising a water-soluble lubricant. 64. The composition of claim 50, wherein magnesium metal and acid are present in amounts sufficient to provide pH 4 and 6. 65. The composition according to claim 50, additionally containing a nutritional supplement. 66. The composition of claim 50, wherein the nutritional supplement is a magnesium salt. 67. The composition according to claim 50, additionally containing a sweetener or flavoring agent. 68. The composition according to claim 50, additionally containing a dye. 69. A kit for producing hydrogen-enriched water for food supplement or pharmaceutical use, comprising a composition according to any one of claims 1 to 68 and a sealable container capable of holding 500 ml to 2 liters of water. 70. The kit of claim 69, wherein the container is a double wall container. 71. A set according to claim 69, wherein the container is capable of holding 500-750 ml of water. 72. A method for producing hydrogen-enriched water, including the steps: contacting the composition according to any one of claims 1 to 68 with water in a container so that the composition breaks down and the magnesium metal and at least one acid react to form H ₂ . 73. The method of claim 72, wherein the pH is less than 7 for at least 1 hour. 74. The method of claim 72 wherein the pH is 4-6. 75. The method of claim 72, wherein the water contains fruit juice. 76. A method of administering hydrogen to an individual, comprising providing the individual with a composition containing hydrogen formed from a composition according to any one of claims 1-68. 77. The method according to paragraph 76, where the composition containing hydrogen is a nutrotical composition or composition for local use. 78. The method of claim 76 or 77 wherein the nutraceutical is a beverage. 79. Composition for obtaining hydrogen-enriched water, containing: metallic magnesium; at least one food acid; And a binder, where the binder is a sugar; where the composition is a tablet, where the composition reacts with the formation of H ₂ as it decomposes on contact with water, and where the part of the composition containing 60-100 mg of magnesium produces from 3-20 mm dissolved and suspended H ₂ when it decomposes into 500 ml of water in an open container. 80. The composition of claim 79, wherein the composition passes a pharmaceutical friability test. 81. The composition of claim 79, wherein the composition disintegrates in less than 2 minutes. 82. The composition of claim 79, wherein the pH of the water remains less than 7 for at least 10 minutes after the composition has been contacted with water. 83. The composition of claim 79 wherein the magnesium metal comprises flakes. 84. The composition of claim 79 wherein the magnesium metal comprises -325 gauge flakes. 85 The composition of claim 79 wherein the magnesium metal is particulate. 86. The composition of claim 79 wherein the magnesium metal is 200 gauge or less. 87. The composition according to paragraph 79, where at least one digestive acid is selected from a group consisting of maleic acid, amber acid, apple acid, fumaric acid, ants, citric acid, ascorbic acid, oxalic acid and wine -ocamic acid, or them mixtures. 88. The composition according to clause 79, where at least one nutritional acid is wine -stoneic acid. 89. The composition according to clause 79, where at least one nutrient acid is apple acid. 90. The composition of claim 79, wherein the at least one food acid is 60 gauge or less. 91. The composition according to claim 79, wherein the amount of at least one food acid is 30-4000 mg. 92. The composition of claim 79, wherein the binder is maltose, dextrose, or lactose. 93. The composition of claim 79, wherein the binder is dextrose. 94. The composition of claim 79, wherein the binder is lactose. 95. The composition of claim 79, further comprising a water-soluble lubricant. 96. The composition of claim 79, wherein the water-soluble lubricant is selected from sodium stearyl fumarate or stearic acid. 97. The composition of claim 79, wherein the water-soluble lubricant is sodium stearyl fumarate. 98. The composition of claim 79, wherein the composition retains a pH of less than 7 7 days after contact with water. 99. The composition according to claim 79, additionally containing a dye. 100. Composition according to claim 79, additionally containing a perfume. 101. The composition of claim 79, wherein the composition is in the form of a bath tablet.