Compositions for producing hydrogen-rich water and other products

Abstract

Compositions for producing hydrogen-rich water, nutraceuticals, cosmetics, pharmaceuticals and other products are provided. In one embodiment, the present invention provides a composition, such as a tablet, comprising magnesium metal, at least one water-soluble acid, and a binder. The magnesium metal and the at least one water-soluble acid are present in an amount sufficient to maintain a pH of less than 7, e.g., at a specific period after the reaction, and an H2 concentration of at least 0.5 mM after the reaction in 50 mL of water in a container, e.g., a sealed or open container, e.g., an H2 concentration of at least 0.5 mM after the reaction in 100 mL of water or an H2 concentration of at least 0.5 mM after the reaction in 500 mL of water. The composition may also include a lubricant.

Description

[0001] This application is a divisional application of the patent application with the application date of July 17, 2017, application number 201780056644.4 (PCT / IB2017 / 001067), and the invention title of "Composition for Producing Hydrogen-Rich Water and Other Products". Technical Field

[0002] The present invention relates to a composition for producing hydrogen-rich water and other products. Background Art

[0003] Molecular hydrogen has been found to have potential therapeutic uses for various disease injuries. For example, H 2 has been demonstrated to be useful as a method for reducing skin wrinkles (J. Photochem. Photobiol. B. 2012; 106:24 - 33), treating atopic dermatitis (Evid. Based Complement. Alternat. Med. 2013; 2013:538673), and as a post-treatment protocol for radiotherapy (Biochem. J., 2012, 442(1); 49 - 56). Hydrogen-rich water is one way to administer molecular hydrogen to a subject. Commonly used electrolytic and base metal methods for producing hydrogen-rich water typically produce an alkaline solution with a low H 2 concentration.

[0004] Producing H 2 (and thus hydrogen-rich water) in ready-to-drink containers has its technical challenges. Devices commonly used to saturate a sufficient volume of water with H 2 are both expensive and largely inefficient. When utilized, according to Henry's law, at SATP conditions, H 2 can dissolve at a maximum concentration of 0.8 mM or 1.6 ppm. To maintain this H 2 concentration for any period of time, the container cannot have any headspace or the beverage must be supersaturated to allow H 2 to dissipate into the headspace to reach equilibrium. As seen with other commercially available products on the market, even when there is no headspace, the level of H 2 in the container will rapidly drop to ~1 ppm and will continue to drop towards 0 ppm, depending on the sealing technology, headspace level, and initial concentration. Some products have little H 2 remaining by the time they reach the consumer. For example, the Japanese government recently evaluated consumer products containing H 2 and found that most had no detectable level of H 2 (http: / / www.kokusen.go.jp / news / data / n-20161215_2.html).

[0005] Therefore, there is a need for new compositions for generating hydrogen-rich water, which maximize the dissolved hydrogen concentration. SUMMARY OF THE INVENTION

[0006] The present invention provides compositions for generating hydrogen-rich water, nutritional products, cosmetics, pharmaceuticals, and other products. In one embodiment, the present invention provides a composition, such as a tablet, comprising magnesium metal, at least one water-soluble acid, and a binder. The amounts of the magnesium metal and at least one water-soluble acid present may be sufficient to maintain a pH below 7, for example, at a specific time period after the reaction, and at least 0.5 mM of H 2 concentration, such as at least 0.5 mM of H 2 concentration after reaction in 50 mL of water or at least 0.5 mM of H 2 concentration after reaction in 100 mL of water or at least 0.5 mM of H

[0007] In another aspect, the present invention provides a composition comprising magnesium metal, at least one water-soluble acid, and a binder, wherein the at least one water-soluble acid has a solubility of at least 0.01 g / mL in water. In certain embodiments, the composition disintegrates in less than 5 minutes, particularly in less than 2 minutes. In certain embodiments, the composition generates at least 0.5 mM of 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 of H 2 after reaction in 100 mL of water or at least 0.5 mM of H 2 after reaction in 500 mL of water. The composition may further comprise a lubricant.

[0008] In certain embodiments of the above aspects, the composition disintegrates in less than 5 minutes, such as less than 2 minutes. In certain embodiments, the disintegrated composition maintains a pH below 7 at 10 minutes after contact with water and generates at least 0.5 mM of 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 of H 2 after reaction in 100 mL of water or at least 0.5 mM of H 2 .

[0009] In another aspect, the present invention provides a composition comprising magnesium metal, at least one acid, and a binder, wherein the composition disintegrates in less than 5 minutes to maintain a pH below 7 at 10 minutes after disintegration and at least 0.5 mM of 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 of H 2or at least 0.5 mM of H after reaction in 500 mL of water 2 .

[0010] In certain embodiments of any of the above aspects, the composition passes a pharmaceutical friability test. In certain embodiments, the pH of the water is less than 7 at 10, 15, 20, 30, or 45 minutes after contact of the composition with water. In certain embodiments, 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 open to the atmosphere. In certain embodiments, the container is closed. In certain embodiments, when the container is closed, the pH remains less than 7 at 7 days after contact with water. In certain embodiments, the magnesium in the composition reacts to produce H as it disintegrates in water 2 , i.e., the disintegration rate and consumption rate of magnesium are substantially the same.

[0011] The amount of magnesium metal is, for example, 5 - 500 mg, such as 5 - 100 mg. The amount of acid is, for example, 30 - 4000 mg, such as 200 - 400 mg. In certain embodiments, the amounts of magnesium metal and acid present are sufficient to maintain the pH between 4 and 6, and / or the amounts of magnesium metal and acid present are sufficient to produce at least 2 mM of H in 50 mL of water in a container, such as a sealed or open container 2 concentration, such as at least 2 mM of H after reaction in 100 mL of water 2 concentration or at least 2 mM of H after reaction in 500 mL of water 2Concentration. In certain embodiments, the magnesium metal comprises flakes, such as -325 mesh flakes. In other embodiments, the magnesium metal is pulverized, such as 200 mesh or smaller. In some embodiments, the at least one acid is an edible acid. Edible acids are, for example, maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, tartaric acid, or combinations thereof. Exemplary edible acids are tartaric acid and malic acid. In some embodiments, the acid is a cosmetic or pharmaceutically acceptable acid. Cosmetic or pharmaceutically acceptable acids 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, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxyethanesulfonic acid, lactic acid, lactic acid, lauric acid, lauryl sulfate, 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, or combinations thereof. Other acids include acetylsalicylic acid and 5-aminosalicylic acid. Examples of binders are mannitol, xylitol, maltose, dextrose, and lactose. Exemplary binders are dextrose and lactose. In certain embodiments, when the acid is tartaric acid, citric acid, 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, such as at least 50 mg.

[0012] The composition may further comprise a nutritional supplement, 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. Exemplary polysaccharides include cellulose and its derivatives, such as methylcellulose or hydroxypropylmethylcellulose, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin. Exemplary lubricants include sodium stearoyl fumarate and stearic acid, especially sodium stearoyl fumarate.

[0013] The present invention also provides a kit, which comprises the composition of the present invention and a sealable container capable of holding 100 mL to 2 L of water, such as 150 - 750 mL of water. In certain embodiments, the container is double-walled.

[0014] The present invention also provides a method for producing hydrogen-rich water by contacting the composition of the present invention with water in a container so that the composition disintegrates and the magnesium metal reacts with at least one acid to produce H 2 at a concentration of at least 0.5 mM H 2 in water and maintaining the pH below 7 at 10 minutes after disintegration at atmospheric pressure and room temperature. In certain embodiments, the water comprises fruit juice, such as fruit juice containing pectin. In other embodiments, H2 The concentration is at least 1 mM. In certain embodiments, the pH present 1 hour after disintegration is less than 7.

[0015] The present invention also provides a method of administering hydrogen to a subject by providing to the subject a composition containing hydrogen generated from the composition (e.g., a tablet) of the present invention. In some embodiments, the composition containing hydrogen is a nutritional product or a topical formulation. In one embodiment, the nutritional product is a beverage.

[0016] The present invention also provides a hydrogen-rich composition, wherein hydrogen gas is dissolved in a carrier at a concentration of at least 0.5 mM, e.g., the pH is less than 7. In some embodiments, the carrier is edible, cosmetic or pharmaceutical grade. In some embodiments, the carrier is an aqueous liquid, cream, lotion, foam, paste or gel. In some embodiments, the composition is a beverage. In certain embodiments, the maximum concentration of hydrogen is 20 mM. In some embodiments, the pH of the composition is 4 - 6. In one embodiment, the pH is 4.6 or lower. In some embodiments, 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 sweetening agent, flavoring agent, coloring agent, fragrance, essential oil or polysaccharide. In some embodiments, the composition contains a binder or a water-soluble lubricant.

[0017] The present invention also provides a composition for generating acidic hydrogen-rich water. In one embodiment, the present invention provides a composition, such as a tablet, comprising magnesium metal, an edible acid and a binder. Generally, the amounts of magnesium metal and edible acid present are sufficient to produce a pH less than 7 and at least 0.5 mM of H 2 . The present invention also provides a kit comprising the composition of the present invention, such as a tablet, and a sealable container capable of holding 200 mL to 2 L of water, e.g., 250 - 750 mL of water. In certain embodiments, the container is double-walled. The present invention also provides a method of generating hydrogen-rich water by contacting the composition of the present invention, such as a tablet, with water in a sealable container to cause the composition, such as a tablet, to disintegrate and the magnesium metal and the acid to react to produce H at a concentration of at least 0.5 mM H 2 in water 2 and a pH less than 7, e.g., a pH between 4 and 6. In certain embodiments, the water includes fruit juice, e.g., fruit juice containing pectin. In other embodiments, the concentration of H 2 is at least 1 mM. The amount of magnesium metal is, for example, 5 - 100 mg. In certain embodiments, the amounts of magnesium metal and edible acid present are sufficient to produce a pH between 4 and 6, and / or the amounts of magnesium metal and edible acid present are sufficient to produce at least 2 mM of H in 500 mL of water in a sealed container2 。In some embodiments, the magnesium metal is in powder form, such as 200 mesh or smaller. In other embodiments, the magnesium metal includes flakes, such as -325 mesh flakes. Edible acids are, for example, selected from 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. The composition may further comprise vitamins, minerals such as magnesium salts, sweeteners, flavorants, water-soluble lubricants, or polysaccharides. Exemplary polysaccharides include methylcellulose, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.

[0018] Definitions

[0019] As used herein, the term "cosmetic" refers to a composition that is applied to all or part of the human body (e.g., hands, face, arms, or legs) in order to cleanse, beautify, enhance attractiveness, or alter appearance.

[0020] As used herein, the term "cosmetically acceptable" refers to a composition having ingredients that are acceptable for topical use on the human body.

[0021] As used herein, the term "nutraceutical" refers to a composition having at least ingredients suitable for human consumption. Optionally, pharmaceutical-grade ingredients may be employed, as described, for example, in "Remington: The Science and Practice of Pharmacy" (22nd Edition), edited by L.V. Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, PA.

[0022] As used herein, the term "passes the friability test" refers to a composition that has a mass loss of at most 1% after 100 rotations in the drum of a friability tester (e.g., from Copley Scientific).

[0023] As used herein, the term "pharmaceutically acceptable" refers to a composition having ingredients that are subject to the drug purity standards of the United States Food and Drug Administration and are also regulated by the standards set forth in the United States Pharmacopeia; this standard is 99.9% pure for a particular ingredient.

[0024] As used herein, the term "subject" refers to any animal that can be treated topically, orally, by inhalation, or intravenously with a composition containing H 2 or used to generate H 2 The animals include fish, reptiles, birds (e.g., chickens, turkeys), and mammals. Mammals that can be treated with the compositions of the present invention include primates (e.g., humans, apes), domestic animals (e.g., cows, pigs, sheep), draft animals (e.g., cows, horses, llamas), and companion animals (e.g., dogs, cats). Detailed implementation mode

[0025] The present invention provides a composition, such as a tablet, which disintegrates in water to produce hydrogen-rich water. By using the composition of the present invention in, for example, an instant drink container, a supersaturated level of H 2 , far exceeding the level achievable by adding pure H 2 gas. Compared with existing compositions, one advantage of the present invention is the ability to produce a hydrogen-rich composition that contains a supersaturated amount of H 2 at atmospheric pressure in an open container. Additionally, the present invention provides a composition that passes the drug friability test but still produces a high level of H 2 . Another advantage of the present invention is that the composition can react quickly, for example, in less than 2 minutes, to produce a usable, such as potable, hydrogen-rich product, the H 2 level of which is significantly higher than that of existing compositions.

[0026] The composition contains magnesium metal (i.e., elemental magnesium), an acid, and conventional binders and / or lubricants. In water or an aqueous carrier, the magnesium metal and the acid react to produce H 2 dissolved in water and magnesium ions. One advantage of the present invention is that the composition contains sufficient acid to maintain an acidic pH during the production of H 2 . When the acid used is insufficient, the pH of the reaction will increase, for example, until the solution becomes alkaline, resulting in the reaction stopping before reaching a high level of H 2 . Without wishing to be bound by theory, at high pH, the production of H 2 will terminate due to passivation caused by hydroxides and carbonates acting as ligands with unreacted magnesium particles. When this occurs, less magnesium metal will react, thereby reducing the available H 2 produced, while leaving an unacceptable level of residual solids from the composition in the container. The use of acid is also beneficial because a low pH, such as 4.6 or lower, helps reduce microbial growth and thus the likelihood of contamination. Therefore, in certain embodiments, the present invention provides a composition that will produce a hydrogen-rich product with an acidic pH during use or storage.

[0027] Magnesium metal

[0028] 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 produce at least 0.1 mmol of H, for example, in at least 50, 75, 100, 125, 150, 175, 200, 225, 250, 500, 750, 1000, 1500, or 2000 mL of a suitable carrier such as water.2 , such as at least 0.5 mmol, 1 mmol, 2 mmol, 3 mmol, 5 mmol or 10 mmol of H 2 . Suitable masses of magnesium metal include 5 - 1000 mg, such as 5 - 500 mg, 5 - 450 mg, 10 - 400 mg, 20 - 350 mg, 30 - 300, 40 - 250 mg, 50 - 200 mg, 60 - 100 mg, or about 70 mg or 80 mg of magnesium.

[0029] The physical form of magnesium, such as size and shape, can be utilized to control the rate of the reaction. The particles can be spherical, spheroidal, granular or flaky. Smaller particles and particles with a higher surface area to volume ratio will react with faster kinetics. Mixtures of various sizes can also be employed. Flaky magnesium has a higher surface area to volume ratio than granular magnesium. In certain embodiments, - 325 mesh flaky magnesium can be employed in the composition. As an alternative or in combination, larger sized magnesium or magnesium with a lower surface area to volume ratio relative to flaky magnesium can be used. For example, - 200 mesh magnesium can be used. In other embodiments, +100, - 100, +200, - 200 (e.g., - 200, +325), - 325 or smaller mesh magnesium is used. In certain embodiments, magnesium is supplied in two sizes, such as - 200 and - 325, with the smaller size accounting for 20 - 50% of the total amount and the larger size being the balance.

[0030] acid

[0031] Any water - soluble acid can be employed in the present invention. The acid can be edible, or of cosmetic or pharmaceutical grade. Examples of edible 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, cyclopentanepropionic acid, digluconic acid, dodecyl sulfuric acid, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid, hemisulfuric acid, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2 - hydroxy - ethanesulfonic acid, lactic 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of α - acids (e.g., α - humulone), polycarboxylic acids, Lewis acids such as AlCl 3or combinations thereof. Other acids include acetylsalicylic acid and 5-aminosalicylic acid. The acid is present in an amount that reacts with magnesium metal when the composition is placed in water and optionally maintains a pH below 7. Preferably, for the duration of typical beverage consumption, e.g., at least 30 minutes or 1 hour, the amount of the selected acid is sufficient to maintain a pH below 6, e.g., between 4 and 6. In certain embodiments, the number of moles of acid protons in the acid is at least 10%, 20%, 30%, 40%, 50%, 75%, or 100% greater than the number of moles of magnesium metal present. Suitable acid masses include 30 - 4000 mg, e.g., 100 - 1000 mg, 50 - 900 mg, 100 - 800 mg, 150 - 700 mg, 200 - 600 mg, 250 - 500 mg, 300 - 400 mg, or about 340 mg of acid. An exemplary edible acid is malic acid. Another exemplary edible acid for use in the compositions of the present invention is tartaric acid. Tartaric acid is highly water-soluble, having a solubility in water of 0.125 g / mL. Acids having a solubility between about 0.01 - 1 g / mL, e.g., between about 0.02 - 0.9 g / mL, between about 0.03 - 0.8 g / mL, between about 0.04 - 0.7 g / mL, between about 0.05 - 0.6 g / mL, between about 0.06 - 0.5 g / mL, between about 0.07 - 0.4 g / mL, between about 0.08 - 0.3 g / mL, between about 0.09 - 0.2 g / mL, between about 0.1 - 0.2 g / mL, between about 0.11 - 0.5 g / mL, or between about 0.12 - 0.3 g / mL are suitable for use in the compositions of the present invention. When a highly water-soluble acid is used in the compositions of the present invention, the composition is capable of rapid disintegration upon contact with water, e.g., resulting in a more complete reaction with magnesium. The benefit of such rapid dissolution is that it allows the pH to remain below 7 on a time scale corresponding to beverage consumption, e.g., 1 - 2 hours. Other such acids, including both edible and cosmetic and / or pharmaceutical grade, are known in the art.

[0032] The physical form of the acid, such as size and shape, can be utilized to control the rate of the reaction. For example, an acid that is solid at room temperature, such as malic acid or tartaric acid, can be processed to control the size of the acid particles used to prepare the compositions of the present invention. Smaller particles and particles with a higher surface area to volume ratio will react with faster kinetics. The ground acid particles can be used in various mesh sizes, such as from 40 mesh to 2500 mesh. Without being bound by theory, it is believed that the dissolution rate of the composition is linearly related to the mesh size. The compositions of the present invention prepared with larger acid particles (e.g., 40 - 60 mesh) dissolve more slowly than those prepared with finer (e.g., 120 mesh to 2500 mesh) acid particles. Mixtures of acid particles of various sizes can also be employed. Acid particles with controllable size can be produced by many different techniques, including but not limited to micronization, ball milling, or tumbling. Other methods for producing acid particles with controllable size are known in the art.

[0033] Binder

[0034] Any binder capable of disintegrating in water can be employed. Examples of binders include sugars such as maltose, dextrose, and lactose, and sugar alcohols such as mannitol and xylitol. Exemplary binders for the compositions of the present invention include lactose and dextrose. Other binders for the compositions are known in the art. The amount of the binder is, for example, 10 - 50% by weight of the composition, such as 20 - 30%. The compositions of the present invention can contain a single binder, such as lactose, or can be made from a combination of two or more binders to control the physical properties of the composition.

[0035] The binder can be edible or of cosmetic or pharmaceutical grade as known in the art, such as those known in Remington (Remington: The Science and Practice of Pharmacy, (22nd Edition) edited by L.V. Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, PA).

[0036] Additional components

[0037] The composition may also contain other ingredients, such as nutritional supplements, sweeteners, flavoring agents, coloring agents, fragrances, essential oils, lubricants, polysaccharides or coatings. The composition of the present invention may contain nutritional supplements, such as vitamins, minerals and / or herbal extracts. For example, the composition may contain magnesium salts, potassium salts or calcium salts. Suitable sweeteners are known in the art, such as sucrose, mannose, sucralose, aspartame, saccharin, stevia, monk fruit extract and acesulfame K. The composition may also contain any food-grade coloring agent, such as FD&C dyes, and / or flavoring agents, such as fruit flavorings. The composition may also contain essential oils, such as grape seed oil, wintergreen oil, lavender oil. Other essential oils are known in the art. The composition may also contain fragrances, such as eucalyptus oil. The composition may also contain polysaccharides, such as pectin, psyllium fiber, cellulose and its derivatives (e.g., methylcellulose or hydroxypropyl methylcellulose), various starches, apple powder, lemon powder, lime powder or grapefruit powder. The polysaccharide may increase the amount of H 2 retained after the reaction. The composition may also contain water-soluble lubricants, such as micronized sodium stearyl fumarate or purified stearic acid, e.g., 5 microns. The composition may also have a water-permeable coating, such as a soluble surfactant, to control the rate of dissolution of the composition. The soluble surfactant coating may be a triblock copolymer, such as poloxamer, e.g., poloxamer 407, or a nonionic polymeric surfactant suitable for pharmaceutical use, such as glucoside. For example, the composition may have a coating that dissolves within 5 minutes, e.g., within 1 minute, to allow the user to close the container before the composition begins to disintegrate and begins to produce H 2 before.

[0038] Previous attempts to prepare effervescent compositions such as tablets using typical lubricants such as sodium lauryl sulfate (as described in U.S. Patent Publication 2016 / 0113865) and sodium stearyl fumarate have proven unsuccessful in preparing rapidly disintegrating tablets. This is due to the use of higher amounts of lubricants required to form the tablets. The use of large amounts of non-micronized lubricants results in slow tablet disintegration times, which further produces excessive undissolved residues and a foul taste in the container. In contrast, the composition of the present invention can use much less lubricant, resulting in faster reaction kinetics, satisfactory residue amounts and a pleasant taste.

[0039] Form of the composition

[0040] The composition may be formed into tablets. The tablets can be of any suitable shape. For example, the tablets can be discs, spheres or ovals. A single tablet typically contains the amount of magnesium and acid required to produce the desired amount of H 2 in a given volume of water, such as 50, 150 or 500 mL. However, a combination of multiple smaller tablets can be employed. For example, the size of the tablets can be set to provide sufficient H 2, for larger volumes, multiple tablets can be used. Since the reaction of magnesium metal with acid will be activated by water, the compositions of the present invention are typically stored in a waterproof package such as foil or plastic. The components of the tablets are also typically non-hygroscopic, but hygroscopic components can be used if the tablets are dry-packed in a waterproof container or wrapper. The tablets can be formed by methods known in the art.

[0041] One consideration in forming the compositions of the present invention into tablets is the physical properties of the tablets, such as friability. Friability is defined as the tendency of a tablet to crumble, break, or fracture after compression or other handling. The friability of the tablets is evaluated using a tumbler and measuring the percentage loss in mass of the tablets after a fixed number of drum rotations around the drum. For a tablet to successfully pass the friability test, the mass of the tablet can only decrease by 1% after 100 rotations in the tumbler. For the compositions of the present invention, the friability is controlled by the type and particle size of the acid used in the composition, the type and particle size of the binder, the type and particle size of the lubricant, and the pressure at which the tablets are pressed in the die. Using particles of a finer mesh size generally results in a highly friable tablet. Thus, tablets made from fine-mesh particles are often made at a higher pressure to ensure that they do not fall apart; this has the effect of making the tablets very hard, thereby reducing the rate at which they can disintegrate upon contact with water. Thus, tablets using a fine-mesh acid can be made from a highly water-soluble acid such as tartaric acid to maintain the hydrogen generation reaction.

[0042] Other forms of the composition can also be employed. For example, the composition can be provided in the form of a powder within, for example, a water-soluble capsule or a water-permeable bag, or in the form of small or large beads such as a bath bomb, or in the form of a film.

[0043] The dissolution time of the composition and the H 2 concentration so measured are controlled by the mass percentage of the binder, the mass percentage and type of the lubricant, the acid-to-magnesium ratio, the physical properties of both the magnesium and the acid such as mesh size, and the physical conditions under which the composition is placed. When contacted with water in a container, the compositions of the present invention typically disintegrate in less than 5 minutes, such as less than 4 minutes, less than 3 minutes, less than 2 minutes, or less than 1 minute.

[0044] The temperature of the water in which the composition is placed will affect how quickly the composition disintegrates. Hot water will cause the composition to disintegrate rapidly, but will not maintain a high concentration of hydrogen. Colder water will increase the solubility of hydrogen in the water, but will not cause rapid disintegration of the composition. A suitable temperature for generating hydrogen from the composition of the present invention is about room temperature, e.g., between 15°C and 25°C, such as 15°C, 16°C, 17°C, 18°C, 19°C, 20°C, 21°C, 22°C, 23°C, 24°C or 25°C, e.g., between 59°F and 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.

[0045] After contact with water, the composition will maintain an acidic hydrogen-rich product, e.g., with a pH below 7, e.g., 4 - 6, for at least a period of time. The acidic pH can be maintained throughout the typical time scale of using the hydrogen-rich product, such as 10 minutes after the composition contacts water. For example, the composition of the present invention maintains a pH below 7 for at least 5 minutes, e.g., 5 - 300 minutes, 10 - 250 minutes, 15 - 200 minutes, 20 - 150 minutes, 25 - 120 minutes, 30 - 100 minutes, 50 - 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 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, e.g., at least 0.5 hour, 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 composition can also maintain a pH below 7 for an extended period of time, e.g., one day, seven days, 30 days or six months after the composition contacts water. Additionally, after this time range, the pH of the hydrogen-rich product may become basic, e.g., above 7.

[0046] For compositions designed as cosmetic additives for showers or baths, the dissolution rate of the tablets is an important consideration. The composition must dissolve in water slowly enough to produce a constant level of H 2Another limiting factor is the thermodynamics of the dissolution reaction, as the reaction is exothermic and produces a small amount of magnesium hydroxide. If the reaction proceeds too quickly, the temperature of the resulting solution may become too hot or too much magnesium hydroxide may be produced; both effects can damage the skin. Adding polysaccharides to the composition has been shown to have an effect on the dissolution rate while maximizing the retention of H 2 maximization. The polysaccharide added can be a fibrous polysaccharide such as cellulose and its derivatives, for example hydroxypropyl methylcellulose (HPMC, also known as hypromellose). As an alternative or in addition, a soluble surfactant such as a triblock copolymer (e.g., poloxamer 407) can be added to slow down the dissolution of the tablet, ensure sufficient consumption of magnesium, and maximize the H 2 length of time dissolved in water.

[0047] The hydrogen-rich liquid used as a cosmetic or beauty spray can have a relatively high acid content, and the resulting composition can further increase the H 2 concentration by taking advantage of the natural pH of the skin of 4.5 - 5.2 (Lambers et al., Int. J. Cosmet. Sci., 2006, 28, 359 - 370). H 2 has been shown to provide numerous benefits to the skin, and using a beauty spray as a cleanser to return the skin to its natural pH can have further health benefits.

[0048] Carrier

[0049] The compositions of the present invention are used by contacting the compositions, such as tablets, with a carrier such as water or other aqueous liquids. The water can be pure, such as deionized water, or can contain other dissolved ions, such as spring water or tap water. The water can also contain other components, for example, it can be fruit juice or contain fruit juice, or can contain other dissolved gases, such as carbonated water, or contain dissolved solids, such as sugar or salt. An exemplary fruit juice is lemon juice.

[0050] Select the volume of the carrier based on the application to be hydrogen-enriched. When using the composition of the present invention to produce a beverage, the volume of the liquid to be hydrogen-enriched (e.g., water or juice) is from about 100 mL to 2 L, such as about 100 mL, about 150 mL, about 200 mL, about 250 mL, about 300 mL, about 350 mL, about 400 mL, about 450 mL, about 500 mL, about 550 mL, about 600 mL, about 650 mL, about 700 mL, about 750 mL, about 800 mL, about 850 mL, about 900 mL, about 950 mL, about 1 L, about 1.5 L or about 2 L. When using the composition of the present invention to produce a cosmetic, the amount of water is from about 50 mL to 500 mL, such as about 50 mL, about 100 mL, about 150 mL, about 200 mL, about 250 mL, about 300 mL, about 350 mL, about 400 mL, about 450 mL or about 500 mL.

[0051] Alternatively, water may be present in a topical carrier such as a cream, lotion, foam, paste or gel such that H 2 can be effectively delivered to the skin. Methods for producing water-soluble topical carriers are well known in the art, such as those described in Remington (Remington: The Science and Practice of Pharmacy, (22nd Edition) edited by L.V. Allen, Jr., 2013, Pharmaceutical Press, Philadelphia, PA) and in the cosmetics industry. During or after the reaction of the composition of the present invention with water, the carrier may be stirred, mixed or agitated to ensure a uniform consistency.

[0052] Container

[0053] Various containers can be used to bring the composition into contact with a certain volume of water. In one embodiment, the container has a lid that can be used to seal the container, for example, shortly after introducing the composition into a certain volume of water. While the reaction proceeds to completion, the sealed container will retain the generated H 2 . Alternatively, H 2 can be generated in an open container. An example of a suitable container is a double-walled, double-gasket stainless steel bottle.

[0054] Method of use

[0055] The compositions of the present invention are used by contacting the compositions, such as tablets, with a carrier that will promote dissolution of the composition. An exemplary carrier is water. Generally, the amount of water used to dissolve the composition is between 50 mL and 2 L, such as 50 mL, 150 mL, 250 mL, 355 mL, 500 mL, 750 mL, or 1 L. The user can add the composition to water or other carrier in a sealable container and allow the reaction to proceed for 1 minute or longer, depending on the temperature of the water, such as 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 reacts in less than 2 minutes. Preferably, the volume of the tablet and water results in 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 between 0.5 - 20 mM, between 1 - 15 mM, or between 5 - 10 mM. Relative to the reaction in the absence of polysaccharide, introducing polysaccharide in the composition, or in water or a carrier such as in fruit juice, can locally increase the concentration of H 2 in the composition 2 .

[0056] As is known in the art, the consumption of hydrogen-rich water helps to treat various conditions, 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 by Ichihara et al. (Med. Gas Res. (2015) 5:12). Thus, a subject suffering from any of these conditions can consume the compositions of the present invention to treat the condition or alleviate one or more of its symptoms.

[0057] In addition, H 2 has been demonstrated to be an effective treatment for a variety of skin diseases. For example, when using the compositions of the present invention to prepare a hydrogen-rich aqueous liquid, the pH of the resulting aqueous liquid can be adjusted to produce a "beauty water" with a pH of 4.5 - 5.5, which has numerous health benefits (Lambers et al., Int. J. Cosmet. Sci. 2006, 28, 359 - 370). This "beauty water" has been used as a carrier base for topical cosmetic ionic magnesium, and its lower pH and H 2 content will effectively promote the absorption of magnesium through the skin (Magnes. Res. 2016; 29(2):35 - 42). In another example, the H2 The product has been demonstrated to be a promising treatment for local skin conditions such as wrinkles, atopic dermatitis, and UV-induced skin burns (Mol. Cell. Toxicol. 2013, 9(1), 15-21). For local indications, the compositions of the present invention can be directly incorporated into dermatological carriers such as creams, lotions, foams, pastes, or gels.

[0058] Generated in situ by H 2 The hydrogen-containing product generated by the in situ generation of H can be used to improve the health of certain livestock, particularly dairy cows. It is believed that H 2 has the potential to increase the useful life and lifespan of dairy cows, thereby increasing milk production.

[0059] The compositions of the present invention can also be used to generate hydrogen gas for inhalation, for example, by breathing in when the gas is evolved from an open container or via a cannula or nasal tube.

[0060] Hydrogen-rich acidic composition

[0061] The compositions of the present invention can be used to manufacture several consumer products, including but not limited to edible foods and nutritional products (e.g., beverages) and skin care products, such as lotions, bath bombs, or shower tablets, to effectively deliver H 2 . In certain embodiments, the hydrogen-rich composition is a beverage in an open container. For topical compositions, the compositions of the present invention can be directly incorporated into pharmaceutical-grade or cosmetic-grade topical carriers such as creams, lotions, foams, pastes, or gels. The topical composition containing H 2 can be immersed, rolled, wiped, or directly sprayed onto the skin.

[0062] For consumer products designed to be ingested into the human body, such as nutritional products, such as beverages, the acids used in the preparation of the compositions of the present invention must be safely consumable, like the edible acids described herein (e.g., malic acid or tartaric acid). The acids used in the compositions of the present invention for manufacturing consumer products designed for topical administration can be any pharmaceutically or cosmetically acceptable acid and its counterion that are considered "generally recognized as safe" for human and veterinary use as defined by the U.S. Food and Drug Administration. Representative acids include acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentanepropionic acid, digluconic acid, dodecyl sulfate, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid, hemisulfuric acid, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxy-ethanesulfonic acid, lactic acid, lactic acid, lauric acid, lauryl sulfate, 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of α acids (e.g., α-humulene), polycarboxylic acids, Lewis acids such as AlCl 3 、or combinations thereof. Other such acids are known in the art.

[0063] The hydrogen-rich water produced by the compositions of the present invention has a dissolved H 2 concentration between 0.5 mM and 20 mM, such as between 1 mM and 15 mM, between 1 and 10 mM, between 1 mM and 4 mM, between 1 mM and 3 mM, between 1 mM and 2 mM, between 1.5 mM and 4 mM, or between 2 mM and 3 mM, such as 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 concentration is between 1 ppm and 3 ppm, between 2 ppm and 4 ppm, between 3 ppm and 6 ppm, between 4 ppm and 8 ppm, between 5 ppm and 10 ppm, between 6 ppm and 12 ppm, or between 5 ppm and 15 ppm.

[0064] The acid content of the composition used to enrich water with hydrogen may be sufficient to maintain a pH below 7, such as below 6, such as between 4 - 6, while consuming a sufficient amount of magnesium. The hydrogen-rich composition may also contain nutritional supplements, such as magnesium salts, sweeteners, flavorings, colorants, fragrances, essential oils, water-soluble lubricants, or polysaccharides.

[0065] Examples

[0066] Example 1

[0067] In this example, hydrogen-rich water was generated by dissolving the following two compositions in separate open containers and the change in the hydrogen concentration released was monitored over time.

[0068] Sample composition #1 - "F6" - was dissolved in 500 mL of water maintained at 17 °C

[0069] 80 mg of magnesium, -325 mesh, flaky

[0070] 120 mg of tartaric acid, 120 mesh

[0071] 200 mg of malic acid, 120 mesh

[0072] 200 mg of dextrose

[0073] 6 mg of sodium stearyl fumarate

[0074] Sample composition #2 - "F1" - was dissolved in 500 mL of water maintained at 17 °C

[0075] 55 mg of magnesium, -200 mesh, 25 mg of crushed magnesium, -325 mesh, flaky

[0076] 340 mg of malic acid, 60 mesh

[0077] 160 mg of lactose

[0078] 6 mg of sodium stearyl fumarate

[0079] The F6 composition containing crushed 120-mesh acid particles (about 1.75 minutes) dissolved faster than the F1 composition with larger 60-mesh granular acid particles (about 3.5 minutes). If the acid in the F6 composition was only crushed to 60 mesh, the dissolution time of the tablets was about 3 minutes. Both the F6 and F1 compositions passed the minimum drug friability test. Further experimental data using crushed tartaric acid particles less than 10 microns instead of 120-mesh particles in the F6 composition gave a tablet dissolution time of 45 seconds. In addition, by using dextrose instead of lactose as a binder, the dissolution time of each tablet was reduced by about 30 seconds while allowing the friability to remain within an acceptable limit.

[0080] The hydrogen concentration obtained after complete disintegration of the F6 composition was 9 ppm. For the F1 composition, the hydrogen concentration after complete disintegration was 3.5 ppm. A similar composition that did not pass the friability test provided a peak hydrogen concentration of 12 ppm after about 75 seconds. All concentration data are the average of about 20 individual tablets for each composition.

[0081] In a second experiment, the dissolution of a composition containing both tartaric acid and malic acid ("F35") and the following ingredients was studied:

[0082] 60 mg of magnesium, -325 mesh, flaky

[0083] 90 mg of tartaric acid

[0084] 150 mg of malic acid

[0085] 150 mg of dextrose

[0086] 6 mg of sodium stearoyl fumarate

[0087] Under the same water conditions as F1 and F6 (e.g., 500 mL of water at 17 °C in an open container), the concentration is 5.3 ppm after a reaction time of approximately 80 - 90 seconds. The measured concentration is the average of approximately 20 tablets.

[0088] Example 2

[0089] An exemplary tablet for producing a hydrogen-rich ready-to-drink beverage contains the following components:

[0090] 30 mg of magnesium, -200 mesh

[0091] 30 mg of magnesium, -325 mesh, flaky

[0092] 90 mg of tartaric acid

[0093] 150 mg of malic acid

[0094] 150 mg of dextrose

[0095] 5.5 mg of stearic acid, 2500 mesh

[0096] Example 3

[0097] A tablet for producing a hydrogen-rich beverage in a closed container contains the following ingredients:

[0098] 55 mg of magnesium, -200 mesh

[0099] 25 mg of magnesium, -325 mesh, flaky

[0100] 310 mg of malic acid

[0101] 100 mg of magnesium malate

[0102] 160 mg of lactose

[0103] 7 mg of sodium stearoyl fumarate

[0104] These ingredients are compressed into tablets using a manual mechanical tableting machine. When dissolved in water in a hermetic 500 mL container, the tablet produces H 2 gas. In a standard soda bottle (500 mL), H 2The concentration reaches 1.6 ppm (0.8 mM) within 15 minutes, 4 ppm (2 mM) within 2 hours, and exceeds 6 ppm (3 mM) within 12 hours. In a double-walled double-gasket stainless steel bottle, the concentration reaches 2.8 ppm (1.4 mM) at 15 minutes, 3.8 ppm (1.9 mM) at 1 hour, and exceeds 7 ppm (3.5 mM) at 12 hours. When the tablet is added to ordinary water, the pH of the final solution is between 4 and 6.

[0105] When using fruit juice (including fruit juices with high pectin content such as lemon, lime, apple, and orange) as the liquid or using fruit juice in addition to the liquid, the concentration of H 2 in the foam at the top of the liquid can exceed 20 ppm (10 mM). With premixed pectin and psyllium husk, an increase in the concentration of H 2 is also observed.

[0106] Example 4

[0107] A tablet configured for use in beverages to produce a high concentration of H 2 comprises the following components:

[0108] 30 mg of magnesium

[0109] 200 mg of malic acid

[0110] A sufficient amount of binder and lubricant

[0111] These ingredients can be compressed into a suitable tablet shape in a tableting die with a diameter of 9 - 11 mm.

[0112] Example 5

[0113] A tablet configured for cosmetic, shower, or bath use comprises the following components:

[0114] 480 mg of magnesium

[0115] 720 mg of tartaric acid

[0116] 1200 mg of malic acid

[0117] A sufficient amount of binder and lubricant to bring the tablet mass to 3600 mg.

[0118] These ingredients can be compressed into a suitable tablet shape in a tableting die with a diameter of 24 mm.

[0119] Example 6

[0120] A second tablet configured for cosmetic, shower, or bath use comprises the following components:

[0121] 240 mg of 325 - mesh magnesium

[0122] 360 mg tartaric acid of 80 mesh (or lower)

[0123] 600 mg malic acid of 80 mesh (or lower)

[0124] A sufficient amount of binder and lubricant to make the tablet mass reach 1800 mg.

[0125] These components can be pressed into a suitable tablet shape in a tableting die with a diameter of 18 mm.

[0126] Example 7

[0127] A tablet configured for use in a beverage or cosmetic spray contains the following components:

[0128] 80 mg - 325 mesh magnesium

[0129] 120 mg tartaric acid of 80 mesh (or lower)

[0130] 200 mg malic acid of 80 mesh (or lower)

[0131] A sufficient amount of binder and lubricant to make the tablet mass reach 600 mg.

[0132] These components can be pressed into a suitable tablet shape in a tableting die with a diameter of 12 mm.

[0133] Example 8

[0134] A tablet configured for use in a beverage or cosmetic spray contains the following components:

[0135] 60 mg magnesium

[0136] 90 mg tartaric acid

[0137] 200 mg malic acid

[0138] A sufficient amount of binder and lubricant to make the tablet mass reach 4500 mg.

[0139] These components can be pressed into a suitable tablet shape in a tableting die with a diameter of 12 mm.

[0140] Example 9

[0141] A tablet configured specifically for use in a cosmetic or beauty spray contains the following components:

[0142] 25 - 40 mg magnesium

[0143] A sufficient amount of acid, in an amount higher than that used for the tablets to produce hydrogen-rich beverages

[0144] A sufficient amount of binder and lubricant.

[0145] These ingredients can be compressed into a suitable tablet shape in a tabletting die with a diameter of 9 mm.

[0146] Example 10

[0147] The advantage of the tablet containing thin flaky magnesium particles is that H 2 molecules are released one at a time. When there is sufficient acid and the mass of magnesium in the tablet is suitable for the volume of liquid to be H 2 saturated (at least 80 mg of magnesium and 300 mg of total acid per 500 mL of liquid), H 2 will be continuously released, first generating H in the picometer size range 2 bubbles, then they coalesce into nanometer-sized bubbles, then micron-sized bubbles, and then larger bubbles. Nanometer-sized bubbles can saturate the aqueous solution to a higher level than bubbles of other sizes and thus can generate a higher H 2 pressure in the liquid. This is because larger bubbles will dissipate from the solution, but nanometer-sized bubbles are more stable and the physicochemical properties of nanometer-sized bubbles are different from those of individual dissolved H 2 molecules, which changes the relationship with Henry's law and the fugacity coefficient of the gas. According to Le Chatelier's principle, the increased pressure will stop the reaction, leaving submicron-sized magnesium flakes suspended in the solution. As H 2 bubbles coalesce and further dissipate, the pressure of the system drops, and an equal amount of magnesium reacts to further generate H 2 .

[0148] When the composition is placed in an open container rather than a sealed bottle, for example, at 1 atmosphere, this continuous reaction will allow the generation of an H 2 concentration greater than 3 ppm, but deliver a constant H 2 supplement to bring the local concentration of H 2 to approximately 9 ppm. By selecting tablet components, such as coatings or binders, the rate of tablet disintegration and subsequent reaction of magnesium with acid can be accelerated to control the reaction kinetics and complete the reaction within no more than 4 minutes, for example, within the range of 1 - 2 minutes.

[0149] Dissolving the composition of the present invention using cold water allows maintaining an increased hydrogen concentration, but also results in a significant slowdown in the tablet dissolution rate, followed by a significant slowdown in the entire hydrogen generation reaction. For example, in water just above the freezing point (1 °C), the tablets of the present invention typically take 4 - 5 minutes to completely dissolve. However, once the water is saturated, the dissolved hydrogen remains at a higher concentration in the water for a longer time. Dissolving the composition of the present invention using hot water will result in a significant increase in the dissolution rate, followed by a faster hydrogen evolution. For example, in hot water, such as above room temperature, the tablets of the present invention typically dissolve completely in 1 minute or less. However, as the temperature increases, the bubble coalescence rate will increase sharply, thus shortening the retention time and reducing the overall stability of the hydrogen-rich water.

[0150] Using current tableting techniques and capabilities, the ideal water temperature range for dissolving tablets made from the composition of the present invention is between 12 - 20 °C, depending on the final composition of the tablets.

[0151] Example 11

[0152] The composition of the present invention, such as tablets, is capable of dissolving and generating semi-stable supersaturated H 2 . Polysaccharides contained within the composition or present in the liquid carrier can form a boundary layer at the surface of the liquid. This boundary layer will prevent the rapid dissipation of the H 2 gas cloud formed by the dissolution of the composition. For example, in a rigid container, adding a pH regulator, such as 2 tablespoons of lemon juice (which contains pectin) or vinegar, will increase the available H 2 concentration. The use of vinegar will result in a higher H 2 concentration throughout the liquid. When water and lemon juice are placed in a standard soda bottle mainly made of polyethylene terephthalate (PET), the concentration of H 2 at the top of the gas cloud will increase by 6 - 7 times. In an open glass bottle with the same water and lemon juice solution, the generated H 2 gas concentration will increase by approximately 20%. When using polysaccharides, a foam will form on the surface of the liquid, which contains a higher H 2 concentration than the rest of the liquid.

[0153] Once the tablet is placed in the container, the open container will be able to rapidly produce a suspension of magnesium nanoparticles. This will increase the reaction rate of generating H 2 . For example, in a tablet that will completely react within 30 to 60 seconds, the bubbles formed at the top of the surface burst violently and result in a measured H 2 concentration of 1.6 ppm.

[0154] For the composition of the present invention, 70 - 90 seconds is the ideal reaction rate, often reaching a supersaturation of 10 ppm in the gas cloud. The measured H2 The concentration appears to decrease linearly with time and, as shown by the data in Table 1, reaches a typical SATP concentration of 1.6 ppm after 8 minutes of dissolution.

[0155] Table 1: H measured after dissolving the composition of the present invention 2 Concentration

[0156] Dissolution time (seconds) <![CDATA[Measured H 2 Concentration (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

[0157] Example 12

[0158] In this example, the H-enhanced water generated by dissolving the composition of the present invention, such as a tablet, in an open container was transferred to a sealable snap-on cap glass bottle and allowed to equilibrate under pressure after further dissolution of the composition. When the sealed bottle was opened, the measured H concentration was 5.3 ppm. 2 In a further experiment, the H-enhanced water generated by dissolving the composition of the present invention, such as a tablet, in an open container was transferred to a sealable PET soda bottle that was modified to include a pressure gauge for measuring the pressure inside the bottle. As the reaction proceeded, the bottle began to pressurize and a headspace was generated inside the bottle as H bubbles formed and then dissipated. After 5 minutes of reaction, the measured bottle pressure was 25 psi and after 30 minutes of reaction, the measured bottle pressure was 45 psi. At this pressure, the measured H concentration was 2.3 ppm. 2 The concentration was 5.3 ppm.

[0159] In a further experiment, the H-enhanced water generated by dissolving the composition of the present invention, such as a tablet, in an open container was transferred to a sealable PET soda bottle that was modified to include a pressure gauge for measuring the pressure inside the bottle. As the reaction proceeded, the bottle began to pressurize and a headspace was generated inside the bottle as H bubbles formed and then dissipated. After 5 minutes of reaction, the measured bottle pressure was 25 psi and after 30 minutes of reaction, the measured bottle pressure was 45 psi. At this pressure, the measured H concentration was 2.3 ppm. 2 In a further experiment, the H-enhanced water generated by dissolving the composition of the present invention, such as a tablet, in an open container was transferred to a sealable PET soda bottle that was modified to include a pressure gauge for measuring the pressure inside the bottle. As the reaction proceeded, the bottle began to pressurize and a headspace was generated inside the bottle as H bubbles formed and then dissipated. After 5 minutes of reaction, the measured bottle pressure was 25 psi and after 30 minutes of reaction, the measured bottle pressure was 45 psi. At this pressure, the measured H concentration was 2.3 ppm. 2 In a further experiment, the H-enhanced water generated by dissolving the composition of the present invention, such as a tablet, in an open container was transferred to a sealable PET soda bottle that was modified to include a pressure gauge for measuring the pressure inside the bottle. As the reaction proceeded, the bottle began to pressurize and a headspace was generated inside the bottle as H bubbles formed and then dissipated. After 5 minutes of reaction, the measured bottle pressure was 25 psi and after 30 minutes of reaction, the measured bottle pressure was 45 psi. At this pressure, the measured H concentration was 2.3 ppm. 2 The concentration was 2.3 ppm.

[0160] The composition in both containers (open bottle and sealed bottle) continued to react with the micron particles. When the H coalesced and dissipated, the pressure contained within the liquid transferred to the headspace, thereby increasing the pressure within the container. Notably, the pressure achieved by transferring the open container liquid to the PET bottle reached and even exceeded the pressure generated by dropping a tablet into the PET bottle and immediately sealing it. According to Le Chatelier's principle, when immediately sealed, the same tablet produced approximately 35 psi due to the reaction stopping, thus also confirming the supersaturation capacity of the composition. 2 The composition in both containers (open bottle and sealed bottle) continued to react with the micron particles. When the H coalesced and dissipated, the pressure contained within the liquid transferred to the headspace, thereby increasing the pressure within the container. Notably, the pressure achieved by transferring the open container liquid to the PET bottle reached and even exceeded the pressure generated by dropping a tablet into the PET bottle and immediately sealing it. According to Le Chatelier's principle, when immediately sealed, the same tablet produced approximately 35 psi due to the reaction stopping, thus also confirming the supersaturation capacity of the composition.

[0161] Example 13

[0162] One variable that exerts control over hydrogen production from the composition of the present invention is the mass of magnesium used to react with the ground acid. The relationship between the mass of magnesium and the dissolved hydrogen concentration is approximately linear - as the amount of magnesium used increases, for a fixed mass of acid, the amount of hydrogen produced increases. Table 2 presents the hydrogen concentration data for various magnesium masses where the acid was ground to a mesh size (~120 mesh) particle size and the dissolution time was approximately 60 - 75 seconds.

[0163] Table 2: H measured after dissolving the composition of the present invention prepared with acid of 120 mesh or less 2 Concentration

[0164] Mass of magnesium (mg) <![CDATA[Measured H 2 Concentration (ppm)]]> 80 9-12 70 N / A 60 4-5 55 3 50 2.6-3

[0165] The effect of the milled acid was also studied by measuring the laser diffraction size distribution of the bubbles generated during the dissolution reaction. Using the milled acid, the generated bubbles exhibited a bimodal distribution. After noise compensation, the first peak was at a diameter of approximately 50 - 60 nm and the second peak was at a diameter of 600 nm. As described in Example 10, compared to bubbles of other sizes, the nanosized bubbles were able to saturate the aqueous solution to a higher level and thus generate a higher H 2 pressure in the liquid, thereby confirming the importance of using the milled acid in the preparation of a composition for enriching water with hydrogen.

[0166] An additional test using tablets made of the milled acid in an open container produced 70 mL of hydrogen within the first 80 - 90 seconds, with a theoretical limit of 80 mL. By the second minute of the reaction, only 6 mL of hydrogen had escaped from the liquid surface in the open container.

[0167] Specifically, the present invention relates to the following clauses.

[0168] 1. A composition comprising:

[0169] Magnesium metal;

[0170] At least one acid; and

[0171] Binder;

[0172] wherein the composition disintegrates in less than 5 minutes and produces at least 0.5 mM of H 2 .

[0173] 2. The composition according to clause 1, wherein the composition passes the pharmaceutical friability test.

[0174] 3. The composition according to clause 1, wherein the composition disintegrates in less than 2 minutes.

[0175] 4. The composition according to clause 1, wherein the pH of the water remains below 7 for at least 10 minutes after the composition contacts the water.

[0176] 5. The composition according to clause 1, wherein the magnesium metal comprises flakes.

[0177] 6. The composition according to clause 1, wherein the magnesium metal comprises - 325 mesh flakes.

[0178] 7. The composition according to clause 1, wherein the magnesium metal is pulverized.

[0179] 8. The composition according to clause 1, wherein the magnesium metal is 200 mesh or smaller.

[0180] 9. The composition according to clause 1, wherein the amount of the magnesium metal is 5 - 500 mg.

[0181] 10. The composition according to clause 1, wherein the at least one acid comprises an edible acid.

[0182] 11. The composition according to clause 10, wherein the at least one edible acid is selected from maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, tartaric acid, or a mixture thereof.

[0183] 12. The composition according to clause 1, wherein the at least one edible acid is tartaric acid.

[0184] 13. The composition according to clause 1, wherein the at least one edible acid is malic acid.

[0185] 14. The composition according to clause 1, wherein the at least one edible acid is 60 mesh or smaller.

[0186] 15. The composition according to clause 1, wherein the at least one acid is a cosmetic or pharmaceutically acceptable acid.

[0187] 16. The composition according to clause 15, wherein the cosmetic or pharmaceutically acceptable acid is 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, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2 - hydroxy - ethanesulfonic acid, lactic acid, lactic acid, lauric acid, laurylsulfuric 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of α - acids (e.g., α - humulone), polycarboxylic acids, Lewis acids, or a combination thereof.

[0188] 17. The composition according to clause 1, wherein the amount of the at least one acid is 30 - 4000 mg.

[0189] 18. The composition according to clause 1, wherein the binder is mannitol, xylitol, maltose, dextrose, or lactose.

[0190] 19. The composition according to clause 1, wherein the binder is dextran.

[0191] 20. The composition according to clause 1, wherein the binder is lactose.

[0192] 21. The composition according to clause 1, further comprising a water-soluble lubricant.

[0193] 22. The composition according to clause 1, wherein the water-soluble lubricant is selected from sodium stearoyl fumarate or stearic acid.

[0194] 23. The composition according to clause 1, wherein the water-soluble lubricant is sodium stearoyl fumarate.

[0195] 24. The composition according to clause 1, wherein the container is open to the atmosphere.

[0196] 25. The composition according to clause 1, wherein the container is closed.

[0197] 26. The composition according to clause 25, wherein the composition maintains a pH below 7 at 7 days after contact with water.

[0198] 27. The composition according to clause 1, wherein the composition reacts to produce H as it disintegrates upon contact with water. 2 .

[0199] 28. The composition according to clause 1, wherein the magnesium metal and at least one acid are present in an amount sufficient to produce at least 2 mM H. 2

[0200] 29. The composition according to clause 1, further comprising a nutritional supplement.

[0201] 30. The composition according to clause 29, wherein the nutritional supplement is a magnesium salt.

[0202] 31. The composition according to clause 1, further comprising a sweetening agent or a flavoring agent.

[0203] 32. The composition according to clause 1, further comprising a coloring agent.

[0204] 33. The composition according to clause 1, further comprising a fragrance.

[0205] 34. The composition according to clause 1, further comprising an essential oil.

[0206] 35. The composition according to clause 1, further comprising a polysaccharide.​

[0207] 36. The composition according to clause 35, wherein the polysaccharide is selected from cellulose and its derivatives, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.

[0208] 37. A composition comprising:

[0209] Magnesium metal;

[0210] At least one water-soluble acid; and

[0211] Binder;

[0212] wherein the composition produces at least 0.5 mM of H 2 when contacted with 50 mL of water in a container at atmospheric pressure and room temperature, and wherein the at least one water-soluble acid has a solubility of at least 0.01 g / mL.

[0213] 38. The composition according to clause 37, wherein the composition passes a pharmaceutical friability test.

[0214] 39. The composition according to clause 37, wherein the composition disintegrates in less than 2 minutes.

[0215] 40. The composition according to clause 37, wherein the magnesium metal comprises flakes.

[0216] 41. The composition according to clause 37, wherein the magnesium metal comprises -325 mesh flakes.

[0217] 42. The composition according to clause 37, wherein the magnesium metal is pulverized.

[0218] 43. The composition according to clause 37, wherein the magnesium metal is 200 mesh or smaller.

[0219] 44. The composition according to clause 37, wherein the amount of the magnesium metal is 5 - 500 mg.

[0220] 45. The composition according to clause 37, wherein the at least one water-soluble acid has a solubility of at least 0.05 g / mL in water.

[0221] 46. The composition according to clause 37, wherein the at least one water-soluble acid has a solubility of at least 0.1 g / mL in water.

[0222] 47. The composition according to clause 37, wherein the at least one water-soluble acid has a solubility of at least 1 g / mL in water.

[0223] 48. The composition according to clause 37, wherein the at least one water-soluble acid comprises an edible acid.

[0224] 49. The composition according to clause 48, wherein the at least one water-soluble edible acid is selected from maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, tartaric acid, or a mixture thereof.

[0225] 50. The composition according to clause 37, wherein the at least one water-soluble edible acid is tartaric acid.

[0226] 51. The composition according to clause 37, wherein the at least one water-soluble edible acid is malic acid.

[0227] 52. The composition according to clause 37, wherein the at least one water-soluble edible acid is 60 mesh or smaller.

[0228] 53. The composition according to clause 37, wherein the at least one water-soluble acid is a cosmetic or pharmaceutically acceptable acid.

[0229] 54. The composition according to clause 53, wherein the cosmetic or pharmaceutically acceptable acid is acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentanepropionic acid, digluconic acid, dodecyl sulfate, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid, hemisulfuric acid, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxy-ethanesulfonic acid, lactic acid, lactic acid, lauric acid, lauryl sulfate, 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of α-acids (e.g., α-humulone), polycarboxylic acids, Lewis acids, or a combination thereof.

[0230] 55. The composition according to clause 37, wherein the amount of the at least one water-soluble acid is 30 - 4000 mg.

[0231] 56. The composition according to clause 37, wherein the binder is mannitol, xylitol, maltose, dextrose, or lactose.

[0232] 57. The composition according to clause 37, wherein the binder is dextrose.

[0233] 58. The composition according to clause 37, wherein the binder is lactose.

[0234] 59. The composition according to clause 37, the composition further comprises a water-soluble lubricant.

[0235] 60. The composition according to clause 37, wherein the water-soluble lubricant is selected from sodium stearoyl fumarate or stearic acid.

[0236] 61. The composition according to clause 37, wherein the water-soluble lubricant is sodium stearoyl fumarate.

[0237] 62. The composition according to clause 37, wherein the container is open to the atmosphere.

[0238] 63. The composition according to clause 37, wherein the container is closed.

[0239] 64. The composition according to clause 63, wherein the composition maintains a pH below 7 at 7 days after contact with water.

[0240] 65. The composition according to clause 39, wherein the composition reacts to produce H 2 .

[0241] 66. The composition according to clause 37, wherein the magnesium metal and at least one water-soluble acid are present in an amount sufficient to produce at least 2 mM H 2 in 500 mL of water.

[0242] 67. The composition according to clause 37, further comprising a nutritional supplement.

[0243] 68. The composition according to clause 67, wherein the nutritional supplement is a magnesium salt.

[0244] 69. The composition according to clause 37, further comprising a sweetening or flavoring agent.

[0245] 70. The composition according to clause 37, further comprising a coloring agent.

[0246] 71. The composition according to clause 37, further comprising a fragrance.

[0247] 72. The composition according to clause 37, further comprising an essential oil.

[0248] 73. The composition according to clause 37, further comprising a polysaccharide.

[0249] 74. The composition according to clause 37, wherein the polysaccharide is selected from cellulose and its derivatives, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.

[0250] 75. A composition comprising:

[0251] Magnesium metal;

[0252] at least one acid; and

[0253] a binder,

[0254] wherein the composition produces at least 0.5 mM of H after contacting with 50 mL of water in a container at atmospheric pressure and room temperature 2 and maintains a pH below 7 at 10 minutes after contact.

[0255] 76. The composition according to clause 75, wherein the composition passes a pharmaceutical friability test.

[0256] 77. The composition according to clause 75, wherein the pH is maintained below 7 at 30 minutes after contact with water.

[0257] 78. The composition according to clause 75, wherein the pH is maintained below 7 at 1 hour after contact with water.

[0258] 79. The composition according to clause 75, wherein the magnesium metal comprises flakes.

[0259] 80. The composition according to clause 75, wherein the magnesium metal comprises -325 mesh flakes.

[0260] 81. The composition according to clause 75, wherein the magnesium metal is pulverized.

[0261] 82. The composition according to clause 75, wherein the magnesium metal is 200 mesh or smaller.

[0262] 83. The composition according to clause 75, wherein the amount of the magnesium metal is 5 - 500 mg.

[0263] 84. The composition according to clause 75, wherein the at least one acid comprises an edible acid.

[0264] 85. The composition according to clause 84, wherein the edible acid is selected from maleic acid, succinic acid, malic acid, fumaric acid, formic acid, citric acid, ascorbic acid, oxalic acid, and tartaric acid or a mixture thereof.

[0265] 86. The composition according to clause 75, wherein the at least one acid is tartaric acid.

[0266] 87. The composition according to clause 75, wherein the at least one acid is malic acid.

[0267] 88. The composition according to clause 75, wherein the at least one acid is 60 mesh or smaller.

[0268] 98. The composition according to clause 75, wherein the at least one acid is a cosmetic or pharmaceutically acceptable acid.

[0269] 99. The composition according to clause 89, wherein the cosmetic or pharmaceutically acceptable acid is acetic acid, adipic acid, alginic acid, aspartic acid, benzenesulfonic acid, benzoic acid, boric acid, butyric acid, camphoric acid, camphorsulfonic acid, cyclopentanepropionic acid, digluconic acid, dodecyl sulfuric acid, ethanesulfonic acid, glucoheptonic acid, glycerophosphoric acid, hemisulfuric acid, heptanoic acid, hexanoic acid, hydrobromic acid, hydrochloric acid, hydroiodic acid, 2-hydroxyethanesulfonic acid, lactic 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, sulfuric acid, tartaric acid, thiocyanic acid, toluenesulfonic acid, undecanoic acid, valeric acid, their stereoisomers, all forms of α-acids (e.g., α-humulene), polycarboxylic acids, Lewis acids, or combinations thereof.

[0270] 100. The composition according to clause 75, wherein the binder is mannitol, xylitol, maltose, dextrose or lactose.

[0271] 101. The composition according to clause 75, the composition further comprising a water-soluble lubricant.

[0272] 102. The composition according to clause 75, wherein the magnesium metal and the acid are present in an amount sufficient to produce a pH between 4 and 6.

[0273] 103. The composition according to clause 75, wherein the magnesium metal and the acid are present in an amount sufficient to produce at least 2 mM H 2 +.

[0274] 104. The composition according to clause 75, the composition further comprising a nutritional supplement.

[0275] 105. The composition according to clause 75, wherein the nutritional supplement is a magnesium salt.

[0276] 106. The composition according to clause 75, the composition further comprising a sweetening or flavoring agent.

[0277] 107. The composition according to clause 75, the composition further comprising a coloring agent.

[0278] 108. The composition according to clause 75, the composition further comprising a fragrance.

[0279] 109. The composition according to clause 75, the composition further comprising an essential oil.

[0280] 101. The composition according to clause 75, wherein the composition further comprises a polysaccharide.

[0281] 102. The composition according to clause 101, wherein the polysaccharide is selected from cellulose and its derivatives such as hydroxypropyl methylcellulose, starch, apple powder, lemon powder, lime powder, grapefruit powder, psyllium husk, and pectin.

[0282] 103. A kit, the kit comprising the composition according to any one of clauses 1 - 102 and a sealable container capable of holding 100 mL to 2 L of water.

[0283] 104. The kit according to clause 103, wherein the container is double - walled.

[0284] 105. The kit according to clause 103, wherein the container is capable of holding 250 - 750 mL of water.

[0285] 106. A method for producing hydrogen - rich water, the method comprising the steps of:

[0286] Contacting the composition according to any one of clauses 1 - 102 with water in a container so that the composition disintegrates and magnesium metal reacts with at least one acid to produce H 2 .

[0287] 107. The method according to clause 106, wherein the pH below 7 is maintained for at least 1 hour.

[0288] 108. The method according to clause 106, wherein the pH is 4 - 6.

[0289] 109. The method according to clause 106, wherein the water comprises fruit juice.

[0290] 110. The method according to clause 106, wherein the H 2 concentration is at least 0.5 mM.

[0291] 111. A method for administering hydrogen to a subject, the method comprising providing to the subject a composition containing hydrogen produced by the composition according to any one of clauses 1 - 102.

[0292] 112. The method according to clause 111, wherein the hydrogen - containing composition is a nutritional product or a topical preparation.

[0293] 113. The method according to clause 111 or 112, wherein the nutritional product is a beverage.

[0294] 114. A hydrogen - rich composition, the composition comprising hydrogen dissolved in a carrier at a concentration of at least 0.5 mM, wherein the pH of the composition is below 7.

[0295] 115. The composition according to clause 114, wherein the carrier is edible or of cosmetic or pharmaceutical grade.

[0296] 116. The composition according to clause 114 or 115, wherein the carrier is an aqueous liquid, cream, lotion, foam, paste or gel.

[0297] 117. The composition according to clause 114, wherein the composition is a beverage.

[0298] 118. The composition according to clause 114, wherein the maximum concentration of hydrogen is 20 mM.

[0299] 119. The composition according to clause 114, wherein the pH is 4 - 6.

[0300] 120. The composition according to clause 114, wherein the pH is 4.6.

[0301] 121. The composition according to clause 114, wherein the composition further comprises a nutritional supplement.

[0302] 122. The composition according to clause 121, wherein the nutritional supplement comprises magnesium ions.

[0303] 123. The composition according to clause 114, wherein the composition further comprises a sweetening agent, flavoring agent, coloring agent, fragrance, essential oil, polysaccharide, binder or water-soluble lubricant.

Claims

1. A composition, the composition comprising: Magnesium metal; At least one acid; and Binder; wherein the composition disintegrates in less than 5 minutes and produces at least 0.5 mM of H upon contact with 50 mL of water in a container at atmospheric pressure and room temperature 2 .

2. The composition according to claim 1, wherein the composition passes a pharmaceutical friability test.

3. The composition according to claim 1, wherein the composition disintegrates in less than 2 minutes.

4. The composition according to claim 1, wherein the pH of the water remains below 7 for at least 10 minutes after the composition comes into contact with water.

5. The composition according to claim 1, wherein the magnesium metal comprises flakes.

6. The composition according to claim 1, wherein the magnesium metal comprises -325 mesh flakes.

7. The composition according to claim 1, wherein the magnesium metal is pulverized.

8. The composition according to claim 1, wherein the magnesium metal is 200 mesh or smaller.

9. The composition according to claim 1, wherein the amount of the magnesium metal is 5 - 500 mg.

10. The composition according to claim 1, wherein the at least one acid comprises an edible acid.