JPH1192388A - Produced solution containing free hydrogen ton - Google Patents

Abstract

PROBLEM TO BE SOLVED: To obtain the subject produced solution easy in production, capable of easily eliminating superoxide anion radicals and useful for medicines by including free hydrogen ions obtained by neutralizing hydroxide ions produced by the electrolysis of an electrolyte solution with a specific acid. SOLUTION: This produced solution containing free hydrogen ions contains hydrogen ions (H<+> ) which are obtained by electrolyzing an electrolyte solution (using e.g. sodium chloride as an electrolytic auxiliary) by the use of inactive electrodes such as platinum electrodes through e.g. a diaphragm (concretely an anion or cation exchange membrane) or the like to produce free hydroxide ions (OH<-> ) on the cathode side, and subsequently neutralizing the produced electrolyte solution with ascorbic acid to produce the free hydrogen ions (H<+> ) (e.g. a compound of formula I is neutralized with OH<-> ions to produce a compound of formula II and the H<+> ). The produced solution is obtained by using e.g. an electrolyte solution having an electrolyte concentration of >=10<-4> mole/L and a free anion and cation concentration of 10<-4> to 10<-2> mole/L as the component A and electrolyzing the solution with an applied direct electric current of 0.25-25 A/L.

Description

DETAILED DESCRIPTION OF THE INVENTION

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a product solution containing free hydrogen ions, and more particularly, to neutralization of an electrolytic product solution having free hydroxide ions generated on the cathode side with ascorbic acid. It relates to a product liquid containing free hydrogen ions in the reaction.

[0002]

2. Description of the Related Art Conventionally, electrolysis of water has been used as an electrolysis aid.
This has been done with electrolytes such as sodium chloride and potassium chloride. Also, electrolysis of water has been performed using a supporting electrolyte that does not actually participate in the reaction, such as sulfuric acid. When a halide is used as in the former case, sufficient ion dissociation is performed, and the electrolyte is completely ionized. Therefore, in the electrolyte, the anion is on the anode, while
The cations diffuse to the cathode, so that the charged ions in the solution serve to move. Therefore, at the anode, a halogen element, for example, a chlorine ion emits an electron, and a chlorine atom changes to a chlorine molecule. In addition, water molecules emit electrons at the anode to generate hydrogen ions and oxygen molecules, and react with chlorine ions diffused and moved from the cathode, resulting in chlorine. When chlorine is formed, the hydrogen ion concentration increases, and part of the chlorine gas becomes hypochlorous acid. On the anode side, an acid solution is formed by the action of hydrochloric acid and hypochlorous acid, and the gas-liquid equilibrium is maintained between the chlorine gas and the oxygen gas under a constant partial pressure. On the other hand, at the cathode, sodium hydroxide is generated by an alkali metal as an electrolyte, for example, sodium ion and hydroxide ion, and hydrogen gas is generated by electrolysis of water. Therefore, on the cathode side, the result shows alkalinity by sodium hydroxide. As a result, the anode side shows acidity and the cathode side shows alkalinity. When a charged membrane is used as the diaphragm, for example, in the case of a cation exchange membrane, only cations in the electrolyte solution move from the anode side to the cathode side, while in the case of an anion exchange membrane, the electrolyte solution Only the anions inside move from the cathode side to the anode side.

[0003] The use of an electrolysis solution for living organisms has been known for a long time. When sodium chloride is used as an electrolyte, hypochlorous acid generated at the anode has a strong bactericidal action. It is used instead of a disinfectant. In addition, in the above-mentioned electrolysis, it is already known that a hydroxyl radical is generated on the anode side, and when used directly on a living body, it has some effect on the biological defense mechanism of the living body, thereby enhancing the immune function. There is also a theory.

On the other hand, for use on the cathode side, tap water is electrolyzed, and the electrolyzed water generated on the cathode side is drunk to suppress abnormal fermentation in the gastrointestinal tract and suppress gastric acid. It is widely used because it can. The alkaline electrolyzed water generated on the cathode side is a hydroxide of an alkali metal, and particularly in the case of calcium, is dissolved in water as calcium hydroxide. Further, water molecules are reduced on the cathode surface, and hydrogen gas is generated. Since the generated electrolyzed water on the cathode side contains a large amount of hydrogen gas, the oxidation-reduction potential is lowered due to the concentration ratio with water, and as a result, the oxidation-reduction potential may reach as high as −300 mV. For these purposes, the electrolyzer is directly connected to the water supply, and the electrolysis product can be collected from both the cathode side and the anode side with a simple operation. Also, in order to indicate the characteristics of the electrolytically generated solution, the oxidation-reduction potential and the hydrogen ion concentration of the solution are used as indices.

[0005] However, in the above-mentioned electrolysis solution on the cathode side, an alkali metal hydroxide and hydrogen gas are known as composition components, and as described above, the indexes are the oxidation-reduction potential and the hydrogen ion concentration. Has been adopted.
In the electrolysis solution on the cathode side, an oxidation-reduction potential is used as an index of reducibility, but the oxidation-reduction potential in the electrolysis solution is determined by the Nernst equation, such as the concentration correlation between hydrogen gas and water. It is determined by the hydrogen ion concentration, and therefore cannot always be an index of reducibility. Furthermore, the electrolysis solution on the cathode side cannot be a scavenger having an action of eliminating superoxide anion radicals as free radicals by hydroxide and hydrogen gas. Similarly, in the anode-side electrolysis solution, an acid such as hydrochloric acid, oxygen gas, and hypochlorous acid are known as constituent components, but as a disinfecting action,
Obviously, hypochlorous acid plays this role.
However, phenomena such as promotion of granulation are difficult to explain with these components, and it is necessary to find an independent system for the healing system.

In vivo, mitochondria in cells undergo oxygen electron reduction, and the reaction proceeds continuously from superoxide anion radical, which is a one-electron reduction of oxygen, to H ₂ O, which is a four-electron reduction state. In the process,
Hydrogen ions and hydroxyl ions are consumed. Among these ion species, hydroxyl ions are said to be involved in the electron transport system. In general, the electrolysis solution generated on the cathode side, when subjected to strong electrolysis, reaches a pH of 11 or more and is difficult to be directly taken into a living body, so that the electrolysis solution cannot be used. However, when strong electrolysis is performed, the concentration of free ions increases. L-ascorbic acid or ascorbic acid sodium is located in the third and second positions,
The latter has a hydroxyl group at the second position, and the reaction of both with an alkali is known. Ascorbic acid is also widely known as a free radical scavenger.

[0007]

SUMMARY OF THE INVENTION The present invention has been made in view of the above circumstances, and an object of the present invention is to provide a method for electrolyzing an electrolyte solution to obtain free ionic species on both electrode sides.
In other words, free hydroxyl ions are generated at the cathode, and free hydrogen ions are generated at the anode, and the free hydroxyl ions and ascorbic acid generated at the cathode side are neutralized, and as a result, free hydrogen ions are generated. Is to generate it. Since the hydrogen ion-containing product solution is generated by a strong electrolysis by a neutralization reaction with the generated electrolysis solution, the high pH electrolysis solution is adjusted to an arbitrary pH and contains free hydrogen ions. It is an object of the present invention to provide such a product liquid.
In general, electrolytes such as sodium chloride dissolve in water, resulting in sodium ions as cations and chloride ions as anions, and at a concentration of about 0.1 M, they are completely dissociated. , The concentrations of both ions are the same. Similarly, in the case of sodium hydroxide or hydrochloric acid, the concentrations of the cation and the anion are also the same, and the former reacts with the acid and the latter with the base, but free hydroxyl ions, which are free ionic species, Free hydrogen ions do not react with acids or bases, only free ion species of the opposite sign or substitution reactions occur, and it is still another object of the present invention to provide free ion water containing extremely stable free ion species. Is the purpose.

[0008]

Means for Solving the Problems To solve the above-mentioned problems, an electrolytic solution is electrolyzed by an inert electrode to generate free hydroxyl ions on the cathode side, and neutralization of ascorbic acid with an electrolytic product solution. It is characterized by containing free hydrogen ions generated in the reaction. In addition, the electrolyte solution is electrolyzed by an inert electrode through a diaphragm, and as a result, a free solution generated by a neutralization reaction between an electrolysis solution in which free hydroxide ions are generated on the cathode side and ascorbic acid is produced. Characterized by containing hydrogen ions. Still further, the membrane is a charged membrane or an uncharged membrane, and the concentration of the electrolyte solution is saturated from 10 ⁻⁴ mol / l,
And the concentration of free ions of both anions and cations is 10 ^-4 to 10 ^-2
mol / l and the DC applied current value is 0.25 to 2
It is in the range of 5 A / l. Although free hydrogen ions have the molecular structure of oxonium ion H ₃ O ⁺ in water, they are free hydrogen ions for convenience in the present invention.

[0009]

BEST MODE FOR CARRYING OUT THE INVENTION The electrolyzed solution containing free ionic species of the present invention uses a platinum electrode as an inert electrode and sodium chloride as an electrolysis aid. As a result, free ions are electroformed on both electrodes. It was made. Here, as the electrolysis assistant, potassium chloride or calcium chloride which is a divalent monovalent electrolyte may be used in addition to sodium chloride which is a monovalent monovalent electrolyte. The inert electrode may be any electrode as long as it is a platinum-based electrode, and it is an absolute condition that it is an irreversible electrode. Further, as the diaphragm, either an anion exchange membrane or a cation exchange membrane can be adopted. Furthermore, a neutral film, which is an uncharged film, can also be used, but a charged film is
Charged membranes are preferred over neutral membranes because they can further enhance ion selectivity. Even a neutral film may be used as long as the pores constituting the film are small. The production of free hydroxyl ions and free hydrogen ions is possible when the concentration of the electrolyte used is in the range of 10 ⁻⁴ mol / l to a saturated state, and the free ion concentration of the anion and cation is 10 ⁻⁴ to 10 ⁻² mol. / L. If the DC applied current value is in the range of 0.25 to 25 A / l, free ions can be generated. When using an anion exchange membrane, the method for analyzing the electrolytic product solution is such that, on the cathode side, the amount of chloride ions moved to the anode side decreases,
As a result, sodium hydroxide and sodium ion form sodium hydroxide, so that the amount of hydroxyl ion can be determined by neutralization titration. The reduced amount of chloride ions may be quantified by ion chromatography.
Neutralization titration and ion chromatography can be quantified with almost the same precision. The total amount of free hydroxide ions and sodium hydroxide hydroxide can be estimated by dividing the product of current and time by the Faraday constant according to Faraday's law. . Free hydroxyl ions can be determined from the difference between the total amount of hydroxyl ions and the amount determined by neutralization titration or ion chromatography. On the anode side, Faraday (F
The free hydrogen ion is determined from the difference between the total amount of hydrogen ion determined by the law of araday) and the amount of hydrogen ion determined by neutralization titration or ion chromatography.
On the anode side, hydrochloric acid and hypochlorous acid can be quantified as hydrogen ions. The electrode reactions occurring on both sides are shown below.

[0010] The reaction at the cathode side ^{_{H 2 0 + e - → 1}} / 2H 2 + OH - (C1) (1) Na + + OH - (C2) → NaOH (2) _{^{where, [OH - (C1)]}} , [OH ^- _(C2)], the total hydroxyl ion concentration, respectively, indicating the hydroxyl ion concentration of sodium hydroxide. _{^{[Cl - (C1)] -}} [Cl - (C2)] = [Cl - (C3)] (3) _{^{where, [Cl - (C1)]}} , [Cl - (C2)], and [Cl ^- _{(C3 )} ]
Indicates the chloride ion concentration before electrolysis, the chloride ion concentration after electrolysis, and the chloride ion concentration moved from the cathode side to the anode side, respectively. _{^{[OH - (C2)] =}} [Cl - (C3)] (4) The reaction at the anode side _{1 / 2H 2 O → 1 /} 4O 2 + H + (a1) + e - (5) Cl - (a1) → ^{_{1 / 2Cl 2 + e - (}} 6) 1 / 2Cl 2 + H 2 O → HOCl + H + (a2) + e - (7) H + (a2) + Cl - (a2) → HCl (8) cathode amount of chlorine ions diffused moved to the anode side from, because it is both electrodes side the same _{^{amount, [Cl - (a1)]}} + [Cl - (a2)] = [Cl - (C3)] (9) Therefore, the anode Then, the electrode reactions (5) and (6) proceed, and (5),
(8) produces hydrochloric acid. The amount of free hydrogen ions is [H ⁺ _(a1) ] + [H ⁺ _(a2) ] − [HOCl] − [HCl] (10) [H ⁺ _(a1) ] is calculated according to Faraday's law.
It is the value obtained by dividing the product of the current and the electrolysis time by the Faraday constant. The reaction between the cathodic electrolysis solution containing free hydroxyl ions and L-ascorbic acid, which is obtained from the equation (4), is as follows. (A) is a reaction formula between L-ascorbic acid and free hydroxyl ions generated during cathodic electrolysis. In the reaction in a high pH region, L-ascorbic acid reacts with the second and third hydroxyl groups. Free hydroxyl ions are substituted.
At this time, free hydrogen ions are generated. (B) is L-
In the reaction between ascorbic acid and sodium hydroxide during cathodic electrolysis, a neutralization reaction occurs at the second and third positions of L-ascorbic acid in a high pH region, and two molecules of water are generated. In (C), one molecule of water is generated by a reaction in a low pH region.

[0011]

The present invention will be described in more detail by way of examples. The present invention is not limited to these examples. Example 1 An anion exchange membrane was used in a rigid vinyl chloride electrolytic cell, and a platinum electrode was used as an electrode, and 400 ml of a 10 ^-1 M sodium chloride solution was placed on each of a cathode side and an anode side.
A direct current of 0.5 A was applied to perform electrolysis for 9 minutes. The concentration of chloride ion and hydroxide ion generated on the cathode side of the produced electrolytic solution was determined by neutralization titration and ion chromatography. In addition, the concentration of chlorine ions and hydrogen ions generated on the anode side was quantified and
The total amount of hydroxyl ions was determined from the formula ay), and the pH was adjusted to 7.0 with L-ascorbic acid. The product solution containing free hydrogen ions was infused into a dog with lymphosarcoma over a period of 24 hours, resulting in a leukocyte count of 55800 / μl to 34500.
/ Μl and the platelet count is reduced from 39000 / μl to 10
Increased to 6000 / μl. Example 2 An anion exchange membrane was used in a hard vinyl chloride electrolytic cell, and a platinum electrode was used as an electrode, and 400 ml of a 10 ^-4 M sodium chloride solution was placed on each of the cathode side and the anode side.
A DC current of 0.1 A was applied to perform electrolysis for 25 minutes. The concentration of chloride ion and hydroxide ion generated on the cathode side of the produced electrolytic solution was determined by neutralization titration and ion chromatography. In addition, the concentrations of chlorine ions and hydrogen ions generated on the anode side were quantified and
aday), the total amount of hydroxyl ions was determined, and the pH was adjusted to 7.0 with L-ascorbic acid. The solution containing free hydrogen ions was applied to dogs with acute renal failure for 72 hours over 72 hours.
As a result of instillation of 0 ml, ALP was 680 to 228 U / m.
The BUN decreased from 10.1 to 4.6 mg / dl, approaching normal values, resulting in a significant improvement in renal failure. By using the free hydrogen ion-containing product solution of the present invention, the renal function of dogs could be restored.
These prove that free hydrogen ions generated by the neutralization reaction between free hydroxyl ions and L-ascorbic acid acted as free radical scavengers.

[0012]

The electrolytic solution containing free hydrogen ions according to the present invention has the following effects because it is configured as described above. 1) Under certain conditions, by electrolyzing the electrolyte solution,
Free ions are generated in both the anion and the cathode, and the free ions do not react with the electrolyte solution composed of the cations and the anions, acids or bases, and are extremely stable. In this case, as long as free ions of the opposite sign do not exist, the active oxygen containing free radicals can easily reach the site where it is localized, and serve as a scavenger. In addition, when ascorbic acid is present in the living body, it replaces the hydrogen ions of the hydroxyl groups at the third and second positions of ascorbic acid and releases free hydrogen ions. As a result, free hydrogen ions and superoxide Reaction with anions causes disproportionation, producing hydrogen peroxide ions. Thus, free hydrogen ions act like superoxide dismutase. As a result, a cell-level repair action can be promoted, and the disease can be improved. 2) The free ions are transported by electrolysis, and the slightly dissociated water molecules are transported as the ions diffuse and move.
That is, by being transported as electrons, an energy balance is established, and ions are generated as ions remaining without being transported. In addition, since the reaction proceeds electrochemically, it can be handled stoichiometrically, and it can be performed extremely easily, and can be produced and manufactured at low cost. It has an excellent effect that it can be manufactured. 3) When strong electrolysis is applied, the amount of generated free ionic species also increases. In particular, in the case of a cathodic electrolysis solution, since it is taken into a living body and used, pH becomes a problem, and by neutralizing with ascorbic acid, And the pH can be adjusted, and suitable conditions can be obtained such that the generated free hydrogen ions can eliminate superoxide anion radicals.
Further, the electrolytic product solution containing free hydrogen ions of the present invention has a remarkable effect such that it can be used as a medicine by increasing the accuracy.

[Brief description of the drawings]

FIG. 1 is a formula showing the reaction between (A) L-ascorbic acid and a hydroxyl group. (B) Formula showing the reaction between L-ascorbic acid and sodium hydroxide. (C) A formula showing a reaction in which L-ascorbic acid reacts with sodium hydroxide to produce a different product from (B).

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[Procedure amendment]

[Submission date] September 22, 1998

[Procedure amendment 1]

[Document name to be amended] Statement

[Correction target item name] 0009

[Correction method] Change

[Correction contents]

[0009]

BEST MODE FOR CARRYING OUT THE INVENTION The electrolyzed solution containing free ionic species of the present invention uses a platinum electrode as an inert electrode and sodium chloride as an electrolysis aid. As a result, free ions are electroformed on both electrodes. It was made. Here, as the electrolysis assistant, potassium chloride or calcium chloride which is a divalent monovalent electrolyte may be used in addition to sodium chloride which is a monovalent monovalent electrolyte. The inert electrode may be any electrode as long as it is a platinum-based electrode, and it is an absolute condition that it is an irreversible electrode. Further, as the diaphragm, either an anion exchange membrane or a cation exchange membrane can be adopted. Furthermore, a neutral film, which is an uncharged film, can also be used, but a charged film is
Charged membranes are preferred over neutral membranes because they can further enhance ion selectivity. Even a neutral film may be used as long as the pores constituting the film are small. The generation of free hydroxyl ions and free hydrogen ions is based on the concentration of electrolyte used being 10 ⁻⁴ mol / l.
To a saturated state, and a free ion concentration of both anions and cations can be generated in a range of 10 ⁻⁴ to 10 ⁻² mol / l. DC applied current value is 0.25-25A
In the range of / l, generation of free ions is possible.
The analysis method of the electrolysis solution is that, when an anion exchange membrane is used, on the cathode side, the amount of chloride ion reduced to the anode side is reduced, and as a result, sodium hydroxide is formed by sodium ion and hydroxide ion. Therefore, the amount of hydroxyl ions can be determined by the neutralization titration method. The reduced amount of chloride ions may be quantified by ion chromatography. Neutralization titration and ion chromatography can be quantified with almost the same precision. In addition, the total amount of free hydroxide ions and sodium hydroxide ions of sodium hydroxide can be estimated from the product of the current efficiency and the value obtained by dividing the product of current and time by the Farady constant according to Farady's law. Further, the electrolyte solution before electrolysis is acidified with a certain concentration of hydrochloric acid, and the consumption amount of sodium hydroxide [OH ⁻ ] ₀ when neutralization titration is performed with a certain concentration of sodium hydroxide is set to ₀ for free hydroxyl ions. The sodium hydroxide consumption [OH ⁻ ] _cathod when the subsequent electrolysis solution was neutralized with the same method from the same pH with sodium hydroxide was determined, and the difference between the former and the latter, [O
From H ⁻ ] _cathod − [OH ⁻ ] ₀ , free hydroxyl ions generated on the cathode side by electrolysis can be determined.
You. The total amount of hydrogen ions on the anode side is Fara
According to dy's law, the product of current and time is given by the Faddy constant
It can be estimated from the product of the divided value and the current efficiency. Ma
Electrolyte solution before electrolysis with a certain concentration of sodium hydroxide
Hydrochloric acid when made alkaline and neutralized with a certain concentration of hydrochloric acid
The amount of consumed [H ⁺ ] _{0 is set} to ₀ for free hydrogen ions,
The subsequent electrolysis solution is treated with hydrochloric acid from the same pH in the same manner.
_Calculate the consumption [H ⁺ ] _anod of hydrochloric acid at the time of neutralization.
Electrolysis from [H ⁺ ] _anod- [H ⁺ ] ₀
The free hydrogen ions generated on the anode side by
Can be. The electrode reactions occurring on both sides are shown below.

[Procedure amendment 2]

[Document name to be amended] Statement

[Correction target item name] 0010

[Correction method] Change

[Correction contents]

[0010] The reaction at the cathode side ^{_{H 2 O + e - → 1}} / 2H 2 + OH - (C1) (1) Na + OH - (C2) → NaOH (2) _{where, [OH- (c1)],} [OH- ( _c2) ] indicate the total hydroxide ion concentration and the hydroxide ion concentration of sodium hydroxide, respectively. ^{_{[Cl - (C1)] -}} [Cl- (C2)] = [Cl - (C3)] (3) ^{_{where, [Cl - (C1)]}} , [Cl - (C2)], and ^[Cl _{- (C3 )]} are respectively the concentration of chlorine ions before the electrolysis, the chloride ion concentration after electrolysis, and the chlorine ion concentration having moved to the anode side from the cathode side. ^{_{[OH - (C2)] =}} [Cl - (C3)] (4) 2 Reaction 1 / _2H at the anode side ^{_{O → 1 / 4O 2 + H}} + (a1) + e - (5) Cl - (al) → 1 / 2Cl ₂ + e ⁻ (6) 1 / 2Cl ₂ + H ₂ O → HOCl + H ⁺ _(a2) + e ⁻ (7) H ⁺ _(a2) + Cl ⁻ _(a2) → HCl (8) Chlorine diffused from the cathode side to the anode side since ion amount is bipolar side the same ^{_{amount, [Cl - (a1)]}} + [Cl - (a2)] = [Cl - (C3)] (9) Therefore, the anode (5), (6) Electrode reaction progresses,
Hydrochloric acid is generated by (5) and (8). Consider current efficiency
Taking into consideration, hydroxide ion amount of liberated ^[OH _-] becomes _{0 (10) (c1) ×} ( current ^{_{efficiency) - [OH -] (c2}} ) = [OH -] cat hod - - [OH] . Free hydrogen ion amount {[H ⁺ _(a1) ] + [H ⁺ _(a2) ]} × (current efficiency)-[HOCl]-[ HCl] = [H ⁺ ] _anod- [H ⁺ ] ₀ (11) [H ⁺ _(a1) ] + [H ⁺ _(a2) ] is Fardy's
According to the law, the product of the current and the electrolysis time is represented by the Faddy constant
It becomes the value which divided. The reaction between the cathodic electrolysis solution containing free hydroxyl ions and L-ascorbic acid, which is obtained from the equation (4), is as follows. (A) is a reaction formula between L-ascorbic acid and free hydroxyl ions generated during cathodic electrolysis. In the reaction in a high pH region, L-ascorbic acid reacts with the second and third hydroxyl groups. Free hydroxyl ions are substituted. At this time, free hydrogen ions are generated. (B) is a reaction between L-ascorbic acid and sodium hydroxide during cathodic electrolysis. In a high pH region, a neutralization reaction occurs at the second and third positions of L-ascorbic acid, and two molecules of water are formed. Is generated. In (C), one molecule of water is generated by a reaction in a low pH region.

 ──────────────────────────────────────────────────続 き Continued on the front page (72) Inventor Takayoshi Hanaoka 1041-2 Ueda, Ueda-shi, Nagano

Claims (4)

[Claims] Claims: 1. An electrolyte solution is electrolyzed by an inert electrode,
A free hydrogen ion-containing production solution characterized by containing free hydrogen ions generated by a neutralization reaction between an electrolysis solution in which free hydroxide ions are generated on the cathode side and ascorbic acid. 2. An electrolyte solution is electrolyzed by an inert electrode through a diaphragm, and as a result, formed by a neutralization reaction between an electrolysis solution in which free hydroxyl ions are generated on the cathode side and ascorbic acid. A product solution containing free hydrogen ions, wherein the product solution contains the obtained free hydrogen ions. 3. The free hydrogen ion-containing product liquid according to claim 2, wherein the diaphragm is a charged membrane or an uncharged membrane. 4. The concentration of the electrolyte solution is 10 ⁻⁴ mol / l.
To a saturated state, the concentration of free ions of both anions and cations is 10 ⁻⁴ to 10 ⁻² mol / l, and the DC applied current value is in the range of 0.25 to 25 A / l. The free hydrogen ion-containing product liquid according to claim 1 or 2, wherein