Contents:

- - I. Summary of the Invention

- - II. Field of the Invention

- - III. Description of Prior Art

- - IV. Demonstration of Novelty Value

- - V. Detailed Description of the Preferred Embodiment

- - VI. Demonstration of Beneficial Effects

- - Claims

- - Abstract

I. Summary of the Invention

The present invention relates to a permanently high hydrogen-containing reducing carbonated bottled drinking water as a product and its automated production and bottling process with gas pressure and liquid level control, in which purified and cooled raw water is first sprayed into a low pressure (e.g. 1-1.5 bar) carbon dioxide gas, and then the carbonated water is sprayed into high pressure (e.g. 8-10 bar) hydrogen gas, and then it is bottled in glass or other special material bottle in an airtight manner, completely filling the space, without gas layer remaining, so a commercially available, easily transportable, explosion risk-free, low mineral content, carbonated, intensive soda water-like, hydrogen-rich water is obtained that retains its ORP value of -340 mV and electron potential of nearly 10.5 rH2 for at least three months from the date of bottling.

II. Field of the Invention

Hydrogen-enriched waters and enrichment processes have been known so far, but these products and processes did not allow for both automated and economical production, long-lasting hydrogen content, and diffusion-free and explosion-risk-free safe bottling.

The activity of hydrogen water prepared with various equipment decreases after its preparation and becomes hydrogen neutral in a few hours. The decrease in activity (i.e., the increase in measurable ORP) can be described by a first-order kinetic linear equation (hydrogen activity [H2] decreases exponentially as a function of time). The ORP of the water prepared with the Lourdes apparatus thus increases along the following linear function: ORP = kt + (ORP)o, ... where (ORP)o is the initial ORP of the water leaving the apparatus in millivolts at time t = 0; t is the time since production in hours; k is the kinetic constant of the decrease in activity, in this device k = 18.6 / h. This value only applies to neutral (pH 6 to 8) waters. Although the alkaline medium stabilizes the hydranions to some extent, the hydrogen activity in the alkaline waters produced by Kangen-type devices decreases rapidly. In these devices the production time, the electrolysis process is very short, the device has a flow-through system, and while max. 10-30 sec, the water passes between the cells, so the binding of hydrogen to the water is less stable.

Example: in water leaving a jug hydrogenator, the pH is 6.3 and the measured ORP = -600 millivolts = -0.60 volts after 30 minutes of hydrogenation. After correction E = - 600 + 200 = -400 millivolts = -0.40Volts. Thus rHa = 33.8E + 2pH = 33.8x (-0.40) + 2x6.3 = -0.92. It is a highly antioxidant water. After twenty-four hours, the ORP of the water rises to ORP = 18.6x24-600 = -154 millivolts while maintaining the pH at 6.5. In this case, rH2 = 33.8x (-0.154 + 200) + 2x6.3 = 14.14. Which is still an antioxidant, but its effect barely exceeds that of the best natural antioxidant mineral waters.

Achieving durability of high hydrogen content is therefore a major challenge because the cost of purchasing fresh water production equipment and the burden of transporting and operating it currently severely limits the commercial availability of hydrogen-rich water for economic reasons.

During manufacturing and bottling, there is a risk that hydrogen will form an explosive mixture with air.

Another problem is that hydrogen from conventional PET bottles evaporates quickly due to its low molecular weight and size, so the hydrogen content decreases in 1-2 days.

The present invention aims to solve the above problems.

With the process of the present invention, hydrogen-rich water can be produced automatically and economically, retaining a hydrogen content of nearly 10.5 rH2, - 340mV ORP for at least three months from bottling, and can be sold commercially without explosion risk, thanks to special bottling, therefore it can be easily accessible to everyone.

HI. Description of Prior Art

1.) The purpose of the process according to JP2009202113 (JP20Q9036) is to produce hydrogen-containing artificial carbonated water having a low ORP by dissolving the gases in water or hot water in such a way that instead of a carbon dioxide gas cylinder, a hydrogen-containing carbon dioxide gas cylinder having an explosion limit or less is used to produce microbubbles or nanobubbles.

In contrast, the process of the present invention is different, e.g., not bubbling the gas into the water but spraying the water into the gas tank and not using a mixed gas, but spraying the water first into carbon dioxide and then into hydrogen, which is much more safe due to the disinfecting effect of carbon dioxide and avoiding risk of explosion, and on the other hand, it is much more economical because it can be easily automated, there is no need for a homogeneous gas mixture that is difficult to produce, and the relative proportions of the two gases in water can be well controlled. Thanks to the unique solution, the hydrogen content becomes durable and a special bottling also takes place.

2.) The hydrogen-containing water production apparatus according to WO2015146969 (PCT/JP2015/058882) comprises a cold water tank in which raw water is stored; a fine bubble generator located in the cold water tank and capable of dispersing fine bubbles in the raw water; a gas supply unit that supplies a mixed gas of hydrogen and carbon dioxide to the fine bubble generator; and a measuring unit capable of measuring the concentration of dissolved hydrogen or carbon dioxide in the raw water in which the fine bubbles are dispersed.

In contrast, the process of the present invention is also different, e.g., not bubbling the gas into the water but spraying the water into the gas tank and not using a mixed gas, but spraying the water first into carbon dioxide and then into hydrogen, which is much more safe due to the disinfecting effect of carbon dioxide and avoiding risk of explosion, and on the other hand, it is much more economical because it can be easily automated, there is no need for a homogeneous gas mixture that is difficult to produce, and the relative proportions of the two gases in water can be well controlled. Thanks to the unique solution, the hydrogen content becomes durable and a special bottling also takes place.

3.) JP2005177724 relates to an apparatus for adjusting the pressure of a mixed gas consisting of hydrogen and nitrogen to 0.25 mpa to 1.0 mpa, the flow rate to 0.1 to 4 liters, and then blowing the raw material into water from a porous element with a pore diameter of 2 to 120 pm and in the form of a fine gas mixture of nitrogen and hydrogen in the form of a fine bubble with a diameter of 2 to 120 pm, an oxidation- reduction potential £400mV and a dissolved hydrogen content of 0,5 to 1,5 ppm.

In contrast, the process of the present invention is different, for example, not the gas is blown into the water, but the water is sprayed in the gas tank, and carbon dioxide is used instead of nitrogen, and not in form of a gas mixture, but separately. Thanks to the new solution, automated bottling can be implemented at a much lower cost, making permanently hydrogen-rich water commercially viable.

4.) The subject of patent application JP2007283280 is the production of hydrogen- rich water using a mixed gas consisting of hydrogen and nitrogen according to the process using the apparatus of the preceding claim.

In contrast, the process of the present invention is different, for example, not the gas is blown into the water, but the water is sprayed in the gas tank, and carbon dioxide is used instead of nitrogen and not in form of a gas mixture, but separately. Thanks to the new solution, automated bottling can be implemented at a much lower cost, making permanently hydrogen-rich water commercially viable.

IV. Demonstration of Novelty Value

Object of the present invention is to enable hydrogen-rich water to be produced automatically and economically which retains hydrogen content of 10.5 rhte with an ORP of -340mV for at least three months, thanks to hermetically sealed, diffusion- free and explosion-proof bottling in glass or other special material bottle, so it can be sold commercially without purchase and operation of a separate equipment.

The present invention makes it possible that the hydrogen-rich water produced during the special manufacturing method retains its hydrogen content three months after bottling, with an ORP value of nearly -340 mV at pH 4.4.

The electron activity of the hydrogen-rich water produced according to the present invention is close to 4 rH2 at opening the bottle, which decreases to nearly 10.5 rH2 three minutes later. All this means that even in the third minute after opening the bottle, we get a strong antioxidant, high hydrogen content and high quality drinking water.

V. Detailed Description of the Preferred Embodiment

According to the present invention, in the first step, the bottling system produces pure, low-mineral water, for example by means of a reverse osmosis water purifier, which reduces the mineral content of the water to about 10-20mg/l and also removes chemical impurities.

The purified water is cooled to a temperature of e.g. about 5-10°C to facilitate better dissolution of the gas.

The cooled water is then sprayed by pump at a pressure of e.g. 8-15 bar in a low pressure (e.g. 1-1.5 bar) CO2 (carbon dioxide) gas and allowed to saturate for e.g. 10 seconds to 30 minutes.

After spraying, the saturation vessel contains approximately 1-2g/3dl of soda water, which is pumped at a pressure of e.g. 10-15 bar into the next saturation vessel, which contains H2 (hydrogen) gas at a high pressure of e.g. 8-14 bar for better absorption, and then it is allowed to saturate for e.g. 10 sec to 30 minutes.

The concentration of H2 (hydrogen) gas results that the ORP of water is -340 mV and the value of rhte is around 10.

It is important that hydrogen does not come into contact with air so it cannot mix in order to avoid risk of explosion.

The purpose of adding carbonated water is twofold, on the one hand to disinfect the water and on the other hand to make bottling safer.

The system is controlled by stable, easily adjustable pressure conditions and automatic water level control, so in practice the bottling (release of hydrogen water) operates, starts and stops the pumps involved in the saturation process, keeping the pressure values within a certain interval and adjusting the saturation tanks the whole process. The system designed in this way allows automatic operation.

The produced water is bottled in glass or other special anti-diffusion bottle so that the liquid almost completely fills the space without a gas layer, leaving only a very small gaseous space above the liquid due to the bubbling of high-pressure gases saturated in the water.

Since H2 (hydrogen) gas would be explosive when mixed with air, this is prevented by that only water and CO2 (carbon dioxide) meet H2 (hydrogen) gas.

During manufacture, the glass must be completely filled with the water-gas mixture so H2 (hydrogen) gas cannot escape.

The bottle is sealed as soon as possible after filling with water, for example at normal atmospheric pressure for the simplest technology.

The volume changes due to the thermal expansion of the liquid are compensated for e.g. by the presence of dissolved carbon dioxide and hydrogen gas.

VI. Demonstration of Beneficial Effects

Hydrogen-enriched waters and enrichment methods have been known so far, but these waters and processes did not allow economical production, long-term hydrogen content and diffusion-free bottling at the same time.

According to the process of the present invention, the water retains the hydrogen content of about 10.5 rH2 for at least three months after bottling, and it is easy to be transported, and it is commercially available to anyone due to its explosion-free bottling.

The purpose of adding carbonated water is twofold: on the one hand, it disinfects the water and protects it from contamination in the future, and on the other hand, it makes bottling safer by eliminating the risk of explosion.

Production is much more economical, because water pumps for water level control make it easy to automate, the r is no need for a difficult-to-produce homogeneous gas mixture, and with this method the ratio of the two gases in the water can be easily controlled between stable values.

Thanks to the water spray system, the condensed water mixture after spraying can be transferred and used almost immediately, which allows continuous operation and eliminates the need for large saturating tanks, thus making the developed technology significantly simpler and cheaper.

The invention makes it possible to easily produce physiologically excellent water that is very high in purity, has excellent solubility (thus very effectively detoxifies the body) and contains only substances that are well known to the human body and are used daily (water, C02 and H2).

Thanks to the process according to the invention, perfectly pure, intense soda-like, highly soluble, antioxidant, medicinal drinking water is produced. The beneficial physiological effects of hydrogen-rich water are confirmed by a number of research findings.

1.) Hydrogen acts as a therapeutic antioxidant by selectively reducing cytotoxic oxygen radicals.

Ohsawa I, Ishikawa M, Takahashi K, Watanabe M, Nishimaki K, Yamagata K, Katsura K, Katayama Y, Asoh S, Ohta S.:

Hydrogen acts as a therapeutic antioxidant by selectively reducing cytotoxic oxygen radicals

Nat Med. 2007 Jun;13(6):688-94. Epub 2007 May 7. https://www.ncbi.nlm nih.goV/pubmed/17486089

2.) Adequate hydration with hydrogen-rich water pre-exercise reduced blood lactate levels and improved exercise-induced decline of muscle function of young athletes.

Kosuke Aoki, Atsunori Nakao, Takako Adachi, Yasushi Matsui, Shumpei Miyakawa: Pilot study: Effects of drinking hydrogen-rich water on muscle fatigue caused by acute exercise in elite athletes

Published online 2012 Jul 12. doi: 10.1186/2045-9912-2-12 https://www.ncbi.nlm.nih.qov/pmc/articles/PMC3395574/

3.) Drinking hydrogen-containing-water reduced hepatic oxidative stress, and significantly alleviated fatty liver in db/db mice as well as high fat-diet-induced fatty liver in wild-type mice. Moreover, drinking hydrogen-containing water decreased levels of plasma glucose, insulin, and triglyceride.

Kamimura N, Nishimaki K, Ohsawa I, Ohta S.:

Molecular hydrogen improves obesity and diabetes by inducing hepatic FGF21 and stimulating energy metabolism in db/db mice.

Obesity (Silver Spring). 2011 Jul; 19(7): 1396-403. doi: 10.1038/oby.2011.6. Epub 2011 Feb 3. https://www.ncbi.nlm.nih.gov/pubmed/21293445)

4.) Drinking 900ml hydrogen-rich water daily for 8 weeks caused significant decreases in the levels of modified low-density lipoprotein (LDL) cholesterol, small dense LDL, and urinary 8-isoprostanes of patients with either type 2 diabetes mellitus (T2DM) or impaired glucose tolerance (IGT). Hydrogen-rich water intake was also associated with a trend of decreased serum concentrations of oxidized LDL and free fatty acids, and increased plasma levels of adiponectin and extracellular-superoxide dismutase.

Kajiyama S, Hasegawa G, Asano M, Hosoda H, Fukui M, Nakamura N, Kitawaki J, Imai S, Nakano K, Ohta M, Adachi T, Obayashi H, Yoshikawa T.:

Supplementation of hydrogen-rich water improves lipid and glucose metabolism in patients with type 2 diabetes or impaired glucose tolerance.

Nutr Res. 2008 Mar;28(3):137-43. doi: 10.1Q16/j.nutres.2008.01.008. https://www.ncbi.nlm.nih.gov/pubmed/19083400 5.) Recent basic and clinical research has revealed that hydrogen is an important physiological regulatory factor with antioxidant, anti-inflammatory and anti-apoptotic protective effects on ceils and organs. Therapeutic hydrogen has been applied by different delivery methods including straightforward inhalation, drinking hydrogen dissolved in water and injection with hydrogen-saturated saline. It is not an overstatement to say that hydrogen's impact on therapeutic and preventive medicine could be enormous in the future.

Chien-Sheng Huang, Tomohiro Kawamura, Yoshiya Toyoda & Atsunori Nakao:

Recent advances in hydrogen research as a therapeutic medical gas

Free Raical Research, September 2010; 44(9): Informa Healthcare; page: 971 https://pubmed.ncbi.nlm.nih.gov/20815764/

6.) Recent evidence suggests that molecular hydrogen has therapeutic value for disease states that involve inflammation. We hypothesized that drinking hydrogen- rich water (HW) daily would protect cardiac and aortic allograft recipients from inflammation-associated deterioration. Drinking Mg-HW or Bu-HW was remarkably effective in prolonging heart graft survival and reducing intimal hyperplasia in transplanted aortas as compared with grafts treated with RW or DW. Furthermore, T cell proliferation was significantly inhibited in the presence of hydrogen in vitro, accompanied by less production of interleukin-2 and interferon-y. Hydrogen treatment was also associated with increased graft ATP levels and increased activity of the enzymes in mitochondrial respiratory chain. Drinking HW prolongs survival of cardiac allografts and reduces intimal hyperplasia of aortic allografts.

Kentaro Noda, Yugo Tanaka, Norihisa Shigemura, Tomohiro Kawamura, Yinna Wang, Kosuke Masutani, Xuejun Sun, Yoshiya Toyoda, Christian A. Bermudez and Atsunori Nakao:

Hydrogen-supplemented drinking water protects cardiac allografts from inflammation- associated deterioration

Transplan International ISSN 0934-0874; Hydrogen water preserves cardiac/aortic allografts page 1 https://pubmed.ncbi.nlm.nih.gov/22891787/

7.) Inhaled hydrogen gas exerts antioxidant and anti-inflammatory effects in rat intestinal transplantation. During the early phase of ischemia-reperfusion injury, hydrogen-enriched solution significantly preserved mucosal graft morphology, diminished graft malondialdehyde levels demonstrating substantial reduction potential and blunted proinflammatory molecular responses (early growth response gene [EGR-1], interleukin [IL]-6, IL-1 b, and inducible nitric oxide synthase) within the reperfused intestinal graft muscularis. During the late phase of ischemia-reperfusion injury, circulating IL-6 protein and lactate dehydrogenase levels were significantly ameliorated in SITxH2 animals, which were associated with a favorable functional outcome in in vivo liquid gastrointestinal transit and recipient solid gastric emptying of chrome steel balls, and marked prevention of the posttransplant associated suppression of in vitro muscarinic jejunal contractility. Reflecting improved graft preservation, hydrogen preloading of grafts increased recipient survival rates from 41% to 80%. Anti-inflammatory and antiapoptotic heme oxygenase-1 was significantly upregulated in the hydrogen-treated graft muscularis but not mucosa before reperfusion. Bettina M. Buchholz, Kosuke Masutani, Tomohiro Kawamura, Ximei Peng, Yoshiya Toyoda, Timothy R. Billiar, Anthony J. Bauer, and Atsunori Nakao:

Hydrogen-Enriched Preservation Protects the Isogeneic Intestinal Graft and Amends Recipient Gastric Function During Transplantation

Basic and Experimental Research; Trasn plantation; Volume 92, Number 9,

November 15, 2011; page: 985 https://pubmed.ncbi.nlm.nih.gov/21956195/

8.) Consumption of molecular hydrogen prevents the stress-induced impairments in hippocampus-dependent learning tasks during chronic physical restraint in mice. Continuous consumption of hydrogen water reduces oxidative stress in the brain, and prevents the stress-induced decline in learning and memory caused by chronic physical restraint. Hydrogen water may be applicable for preventive use in cognitive or other neuronal disorders.

Nagata K, Nakashima-Kamimura N, Mikami T, Ohsawa I, Ohta S.:

Consumption of molecular hydrogen prevents the stress-induced impairments in hippocampus-dependent learning tasks during chronic physical restraint in mice. Neuropsychopharmacology. 2009 Jan;34(2):501-8. doi: 10.1038/npp.2008.95. Epub 2008 Jun 18. https://www.ncbi.nlm.nih.gov/pubmed/18563058)