JP6489378B2 - Method for producing low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate - Google Patents

Description

  The present invention relates to a method for producing a mixed aqueous solution of nickel sulfate and cobalt sulfate having a low chlorine concentration by dissolving a mixture containing at least chlorine, nickel hydroxide, and cobalt dioxide. Impurities are further removed from the mixed aqueous solution of nickel sulfate and cobalt sulfate obtained in (1) by a known method to obtain high-purity nickel sulfate.

  "High-purity nickel sulfate" with low impurity concentration and high nickel purity is used as a general plating material, electroless plating material for hard disks, catalyst materials, materials for electronic parts such as capacitors and inductors, materials for batteries, etc. It is used.

  Recently, the demand for hybrid batteries, electric vehicles, electronic devices such as mobile communication devices and personal computers, nickel metal hydride batteries and lithium ion batteries used in power storage facilities, that is, secondary batteries, has been accelerating. High purity nickel sulfate is used as a raw material for the positive electrode material of these secondary batteries.

There are two types of high purity nickel sulfate products that are shipped in the form of an aqueous solution and those that are shipped in the form of crystals obtained by concentrating, crystallizing, dehydrating and drying the aqueous solution.
Mainly, as materials for electronic parts and batteries, high-purity nickel sulfate aqueous solution with a lower impurity content has been required. Cation constituent elements such as iron, copper and zinc and negative ions such as chlorine A high-purity material that does not contain an ion constituent element is desired, and a manufacturing process therefor has been developed.

As a method for obtaining this high-purity nickel sulfate aqueous solution, for example, there is a method in which high-purity nickel produced through a process such as electrowinning is dissolved in sulfuric acid.
However, a method using high-purity nickel, which has already been obtained with a large amount of energy and labor, using a large-scale apparatus in the manufacturing process is not an advantageous method in view of energy and cost.

Therefore, a method of obtaining a high-purity nickel sulfate aqueous solution in the process of separating and concentrating nickel from mineral resources or secondary resources is advantageous.
In general, a raw material containing nickel is dissolved in sulfuric acid, and impurities such as iron, copper, and cobalt in the obtained crude nickel sulfate aqueous solution are removed.
In the case of crystals, after removing impurities, the aqueous solution is concentrated by heating to evaporate, followed by cooling to precipitate nickel sulfate crystals.

In order to produce high-purity nickel sulfate, it is of course important to dissolve the raw materials and to set the conditions of the crystallization process for precipitating the crystals, but it is better to reduce the impurities in the nickel sulfate aqueous solution before crystallization. is important.
Usually, the raw material for producing nickel sulfate contains impurities such as iron, copper, and zinc in addition to nickel, and these impurities are leached into the solution together with nickel when the raw material is dissolved.

In order to produce high-purity nickel sulfate, it is necessary to remove these cationic constituent elements from the solution by some method. However, if the anionic constituent elements such as chlorine are not completely removed, high-purity nickel sulfate is required. An aqueous solution cannot be produced.
Accordingly, various methods such as precipitation, solvent extraction, and ion exchange have been proposed as methods for removing cation constituent elements, and they can be removed from a crude nickel sulfate aqueous solution relatively easily.
On the other hand, anion constituent elements are generally difficult to remove. In particular, once chlorine ions are mixed into the solution, it is practically very difficult to remove them.

By the way, in nickel smelting, nickel mats mainly composed of nickel sulfide such as Ni ₃ S ₂ obtained by a dry smelting method are produced.
Furthermore, in recent years, the reserves are abundant and close to the surface of the earth. Therefore, nickel oxide ore of low nickel grade that can be mined relatively easily is used as a raw material, and mixed sulfides of nickel and cobalt by a hydrometallurgical process. (Hereinafter, sometimes referred to as mixed sulfide) has been produced.

A method for refining nickel and cobalt using the above nickel mat or mixed sulfide as a raw material, that is, as a nickel hydrometallurgical process, leaching nickel mat or mixed sulfide using the oxidizing power of chlorine gas, A method for removing impurities and commercializing the leached nickel ions and cobalt ions as electrolytic nickel and electrolytic cobalt by electrolytic extraction has been put into practical use.
Here, in the process of removing impurities from the leaching solution, a mixture containing nickel hydroxide containing a trace amount of lead oxide and cobalt hydroxide is generated.
This mixture is dissolved in sulfuric acid and used as a raw material for high-purity nickel sulfate.

This mixture was obtained by injecting chlorine gas into a nickel chloride aqueous solution in which the raw material was leached with chlorine gas and oxidizing it, so that some metals were precipitated as chlorine-containing compounds, and further, chlorine ions In some cases, a mother liquor containing sucrose adheres, and the resulting mixture contains chlorine at a high concentration.
Accordingly, when such a mixture is dissolved in the high-purity nickel sulfate production process, chlorine is also mixed together with nickel. Therefore, efficient removal of chlorine ions is important in low-chlorine nickel sulfate production.

  In Patent Document 1, a slurry of a mixture containing at least chlorine, nickel hydroxide, and cobalt hydroxide is prepared, and the temperature of a solution obtained by adding sulfuric acid to the slurry is set to 60 ° C. or higher, and the pH is set. A method for producing a low chlorine nickel cobalt sulfate solution is disclosed in which the solid components of a slurry are dissolved while being controlled to be 2.0 or less to remove chlorine.

Patent Document 2 discloses a low chlorine concentration in which starch is slurried, sulfuric acid having a concentration of 50% by weight or more is added to the prepared slurry, the pH is adjusted to a range of 0 to 2, and gas is blown into the slurry. A method for producing a mixed sulfuric acid aqueous solution of nickel and cobalt is disclosed.
However, in order to blow in gas, it is necessary to provide a gas blowing device in the melting device, and the equipment cost and the operating cost for gas blowing increase, and the gas blowing time is required, so the melting time also increases. , Has a problem that its operating efficiency is reduced.

In Patent Document 3, an aqueous solution containing cobalt ions is added to a slurry containing nickel hydroxide obtained from a solution obtained by removing cobalt, and then sulfuric acid is added to the slurry to dissolve. A method for producing a low-chlorine nickel sulfate / cobalt solution in which chlorine content is removed by heating is disclosed.
However, adding cobalt leads to an increase in cost for removing cobalt in the subsequent process. Further, since it is necessary to repeat cobalt, there is a disadvantage that the time required for commercialization of cobalt becomes long.

  The techniques disclosed in these patent documents have been improved to the method described in Patent Document 2 or Patent Document 3 on the basis of the method described in Patent Document 1, but in recent years, the technology for the aqueous solution of nickel sulfate has been improved. The demand for purification, that is, a nickel sulfate aqueous solution having a lower impurity concentration has been increasing, and further improvement has been demanded.

JP 2000-203848 A JP 2006-045019 A JP 2012-001414 A

  Therefore, the present invention has been devised in view of the above-mentioned problems of the prior art, and a slurry containing at least chlorine, nickel hydroxide, and cobalt hydroxide is slurried, and sulfuric acid is added to the prepared slurry. Is added to dissolve the solid components in the slurry, and a mixed aqueous solution of nickel sulfate and cobalt sulfate from which the contained chlorine content has been removed is produced without any particular increase in cost and reduction in efficiency. An object is to provide a method for producing a mixed aqueous solution of nickel sulfate and cobalt sulfate having a low chlorine concentration.

  In order to achieve the above-mentioned object, the present inventors slurried a mixture containing at least chlorine, nickel hydroxide, and cobalt hydroxide, and added sulfuric acid to the prepared slurry to add a solid component in the slurry. As a result of earnestly examining the conditions for producing a mixed aqueous solution of nickel sulfate and cobalt sulfate from which the contained chlorine content has been removed and focusing on the slurry concentration, the slurry concentration is 360 g / L or less. As a result, it was found that a mixed aqueous solution of low-chlorine nickel sulfate and cobalt sulfate can be produced efficiently, and the present invention has been completed.

That is, the first invention of the present invention is a mixture containing at least chlorine, nickel hydroxide and cobalt dioxide , wherein the mixture contains 5 to 10% by weight of chlorine and 35 to 60. Containing 1% by weight of nickel and 1-10% by weight of cobalt , adding a slurry aqueous solution to the mixture to form a concentration-adjusted slurry having a slurry concentration of 360 g / L or less, and then adding sulfuric acid to the concentration-adjusted slurry The dissolved solution for dissolving the solid component of the slurry prepared in this manner is maintained at a temperature of 60 ° C. or higher and the pH of the dissolved solution is controlled to 2.0 or lower to dissolve the solid component of the concentration adjusting slurry. To obtain a mixed aqueous solution of nickel sulfate and cobalt sulfate with a low chlorine concentration by removing chlorine contained in the slurry. Is the method.

  The second invention of the present invention is a method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate, characterized in that the slurry concentration of the concentration adjusting slurry in the first invention is 300 to 360 g / L. It is.

  The third invention of the present invention is characterized in that the solid component of the concentration-adjusted slurry is dissolved by controlling the pH of the solution in the first and second inventions to be maintained at 1.5 or lower. This is a method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate.

  According to the method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate of the present invention, a mixed aqueous solution of nickel sulfate and cobalt sulfate having a low chlorine concentration of less than 200 mg / L without any particular increase in cost and efficiency. Can be produced, and has an industrially significant effect.

It is the figure which showed the relationship between slurry concentration and solution chlorine concentration. It is the figure which showed the relationship between the slurry density | concentration and solution chlorine concentration in an Example and a comparative example.

  In the present invention, a mixture containing at least chlorine, nickel hydroxide, and cobalt hydroxide is slurried, and the temperature of a solution obtained by adding sulfuric acid to the prepared slurry is set to 60 ° C. or higher, and the pH of the solution is 2 A method for producing a mixed aqueous solution of nickel sulfate and cobalt sulfate in which the solid component of the slurry is dissolved and the chlorine content is removed while controlling the slurry to be 0.0 or less, and the slurry of the slurry to which sulfuric acid is added The concentration is set to 360 g / L or lower, which is lower than the conventional one.

  First, as one embodiment of the present invention, a high-purity nickel sulfate obtained by dissolving a mixture containing at least chlorine, second nickel hydroxide, and second cobalt hydroxide obtained in a hydrometallurgical process of nickel in sulfuric acid. The present invention will be described by taking as an example the case where it is used for the production of.

[Nickel hydrometallurgical process]
In nickel smelting, for example, nickel sulfide obtained by melting nickel sulfide ore in a smelting furnace, nickel sulfide obtained by adding sulfur to nickel oxide ore and melting in an electric furnace, so-called dry smelting Nickel mats based on nickel sulfide such as Ni ₃ S ₂ obtained by the above method are produced.

  On the other hand, nickel oxide ore of low nickel grade is subjected to pressure acid leaching, and impurities such as iron are removed from the pressure acid leaching solution, and then, for example, hydrogen sulfide gas is converted into nickel ions and cobalt ions by wet sulfidation reaction. The mixed sulfide which has obtained sulfides, such as NiS, as a main component by blowing in in the containing leachate is also produced.

A method for refining nickel and cobalt using the above nickel mat or mixed sulfide as a raw material, that is, as a nickel hydrometallurgical process, leaching nickel mat or mixed sulfide using the oxidizing power of chlorine gas, A method for removing impurities and commercializing the leached nickel ions and cobalt ions as electrolytic nickel and electrolytic cobalt by electrolytic extraction has been put into practical use.
In this method, mixed sulfide is repulped into an aqueous chloride solution and then chlorine gas is blown into the slurry to leach nickel and cobalt into the aqueous chloride solution to form a chlorine leachate. The leaching solution containing divalent copper chloro complex ions as an oxidizing agent is brought into contact with the crushed nickel mat, and the substitution reaction between copper and nickel is performed to replace nickel in the nickel mat with the chlorine leaching solution. It leaches to form a replacement leaching final solution.

The substitution leaching final solution obtained by this substitution leaching is sent to a liquid purification step comprising a deironing step, a solvent extraction step, a deleading step, and a dezincing step.
First, in the deironation process, chlorine gas as an oxidant and nickel carbonate slurry as a neutralizing agent are added to the substitution leaching final solution to generate a precipitate mainly composed of ferric hydroxide, thereby replacing A deiron-free final solution that has been subjected to the treatment for removing iron in the final leach solution is obtained.
Since the pH of the solution during the reaction of this iron removal step is about 2.0 to 2.5, only iron is selectively removed from the solution in this step.

  In the next solvent extraction step, tri-normal-octylamine (TNOA), which is an amine-based extractant, is mixed and brought into contact with the obtained deironated final solution, whereby cobalt, copper, zinc, and iron are extracted from the aqueous phase. An extraction residual liquid (aqueous phase) containing nickel from which cobalt, copper, zinc and iron have been removed is obtained by shifting to the organic phase.

  In the deleading process, similarly to the deironing process, chlorine gas is added as an oxidizing agent, nickel carbonate slurry is added as a neutralizing agent, and the lead in the extraction residual liquid after solvent extraction is removed as lead oxide. Since it produces a deleaded final solution and the pH in the deleading process is controlled to 4-5, a part of nickel also forms a precipitate as a trivalent hydroxide, and the extraction residue after solvent extraction Cobalt remaining in a minute amount in the liquid also forms a precipitate as a trivalent hydroxide.

The precipitate obtained in this deleading step (hereinafter sometimes referred to as deleaded starch) is at least chlorine and trihydric nickel hydroxide, nickel hydroxide [Ni (OH) ₃ And cobaltous hydroxide [Co (OH) ₃ ], which is a hydroxide of trivalent cobalt, is sent to a high-purity nickel sulfate manufacturing process, and sulfuric acid is used as a raw material for the high-purity nickel sulfate. It is dissolved in.

  On the other hand, the deleaded final solution after deleading is sent to the dezincing step, and in the dezincing step, a small amount of zinc chloro complex ion of about 0.1 mg / L remaining in the deleading final solution is weakly basic. A nickel chloride aqueous solution from which impurities are removed by adsorption to an anion exchange resin is obtained.

  The nickel chloride aqueous solution from which impurities have been removed through the liquid purification step as described above is sent to the electrolysis step after pH adjustment, and electronickel is produced by electrowinning.

This method is simple and realizes efficient and economical production such as reusing chlorine gas generated by electrowinning for leaching.
Moreover, about the cobalt isolate | separated by the solvent extraction process, the further impurity removal is performed by the process route different from nickel, and it is commercialized as an electric cobalt by electrowinning.

[Production Method of Low Chlorine Concentration Mixed Aqueous Solution of Nickel Sulfate and Cobalt Sulfate of the Present Invention]
The present invention can be applied to the sulfuric acid dissolution step of the deleaded starch in the “nickel hydrometallurgical process”.
A mixture containing at least chlorine, nickel hydroxide and cobalt dioxide, that is, deleaded starch, which is the basis of the present invention, is converted into water (including pure water) and cleaning liquid discharged in each step. Slurry using an aqueous solution having a low chlorine concentration such as a low-concentration nickel sulfate aqueous solution as a slurry solution, and adding the sulfuric acid to the prepared slurry, the temperature of the solution is 60 ° C. or higher, and the pH is 2.0 or less. A method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate in which a mixture (existing as a solid component in a slurry) is dissolved while removing the chlorine component while controlling so as to be known is known from Patent Document 1 As described above, the oxidation action of nickel hydroxide and cobalt hydroxide during acid dissolution is utilized.

That is, when nickel hydroxide containing chlorine is dissolved in sulfuric acid, nickel is dissolved in the solution according to the following formula (1), and chloride ions are oxidized to generate chlorine gas.
As a result, the chlorine ions contained in the liquid are removed as chlorine gas because the chlorine contained in the deleaded starch has dissolved in the liquid.

  The reaction of cobaltous hydroxide and chloride ions proceeds in the same manner as the above formula (1) (see the following formula (2)).

As can be seen from the formulas (1) and (2), the lower the pH at the time of dissolution, the more convenient the reaction proceeds to the right and the chlorine removal is performed efficiently.
Specifically, the chlorine concentration in the solution can be reduced to 0.5 g / L or lower by adjusting the pH to 2.0 or lower.
More preferably, the pH is 1.5 or less.

By the way, the lower limit of the pH of the solution is not particularly limited, but is preferably 0.5 or more.
The reason is that it is necessary to remove impurities in the solution in a later step, and neutralization treatment is required in any method such as neutralization precipitation method, solvent extraction method, sulfurization method, etc. This is because if the pH is lowered too much, the consumption of the neutralizing agent increases.
Increasing the amount of neutralizing agent used causes not only an increase in drug cost but also an increase in nickel loss, for example.

In addition, the solubility of chlorine gas in the aqueous solution decreases with increasing temperature.
Therefore, dissolution of deleaded starch at a high temperature is advantageous not only for increasing the dissolution rate of nickel and cobalt and increasing the recovery rate, but also for efficiently discharging generated chlorine into the air.
Therefore, the temperature of the solution is preferably 60 ° C. or higher. In addition, since the temperature of a solution is so high that it is desirable for the removal of chlorine, there is no upper limit in particular in the temperature of a solution, but about 100 degreeC is practical from the surface of energy cost or equipment management.

Conventionally, in dissolving sulfuric acid in this deleaded starch, the higher the slurry concentration, the better. Specifically, 300 to 800 g / L, more preferably 400 g / L or more is more preferable.
On the other hand, in this invention, this slurry density | concentration is 360 g / L or less, More preferably, it is 300-360 g / L, and is controlled to a lower level than before.

  In the present invention, the sulfuric acid dissolution step using the deleaded starch is a batch processing step, and a predetermined amount of the deleaded starch slurry is received in the dissolution tank, and the amount of nickel and cobalt in the deleaded starch is received. A predetermined amount of sulfuric acid corresponding to the above is added to maintain the pH at the end of the dissolution reaction at a prescribed control value.

FIG. 1 is a graph showing the relationship between slurry concentration and dissolved solution chlorine concentration.
From FIG. 1, even if the amount of sulfuric acid added is an amount commensurate with the amount of nickel and cobalt in the deleaded starch, that is, even when an operation for maintaining the pH at the end of the dissolution reaction at a prescribed control value is performed, It can be seen that the dissolved solution chlorine concentration depends on the slurry concentration, and the chlorine concentration increases as the slurry concentration increases.
It is estimated that this is because when the slurry concentration is high, the viscosity of the slurry becomes high and reaction failure is likely to occur. Alternatively, it can be estimated that this is because the viscosity of the slurry increases and the chlorine gas is not sufficiently discharged.
Therefore, the slurry concentration is preferably 360 g / L or less. Furthermore, it is more preferable that it is 300-360 g / L.

  When the slurry concentration is less than 300 g / L, the nickel concentration of the solution is lowered, so that the efficiency is lowered in the post-process for removing impurities in the solution and the processing cost is increased. In the concentration and crystallization process, there is a problem that the energy consumption for concentration increases and the processing cost increases, and if the slurry concentration is less than 300 g / L, no further chlorine removal effect can be obtained. When using a slurry concentration of less than 300 g / L, lead starch is dissolved in consideration of the above problem.

[High-purity nickel sulfate production process]
In the solution obtained by dissolving the deleaded starch of the present invention with sulfuric acid, undissolved deleaded starch remains, and in order to eliminate it, sulfite gas as a reducing agent is blown. To complete dissolution.
As a result of this complete dissolution, that is, reduction dissolution, the resulting mixed aqueous solution of nickel sulfate and cobalt sulfate is sent to the next deironing step.

In the next iron removal step, oxidation is performed by blowing air, neutralization is performed by adding a slaked lime slurry of a neutralizing agent, and iron in the mixed aqueous solution of nickel sulfate and cobalt sulfate is secondly oxidized. Precipitate as iron.
The iron removal final solution obtained in the iron removal step is sent to the next solvent extraction step.

  In this solvent extraction step, an acidic extractant such as 2-ethylhexylphosphonic acid mono-2-ethylhexyl phosphonate extracted beforehand is used as an organic phase, while a deiron-containing final solution containing impurities is brought into contact as an aqueous phase so that nickel can be removed. Impurity elements such as cobalt extracted preferentially in the acidic extractant and nickel in the acidic extractant are replaced preferentially to produce a high-purity nickel sulfate aqueous solution from the deironated final solution.

The high-purity nickel sulfate aqueous solution obtained in this solvent extraction step is a low chlorine concentration nickel sulfate aqueous solution, which is shipped as an aqueous solution as a raw material for electronic component materials and battery materials, or in a crystalline state Will be commercialized.
Moreover, when manufacturing the crystal | crystallization of high purity nickel sulfate, the high purity nickel sulfate aqueous solution obtained at the solvent extraction process is sent to the following crystallization process.
In the crystallization step, a high-purity nickel sulfate crystal is produced by concentrating and crystallizing a high-purity nickel sulfate aqueous solution with a crystallizer, and further dehydrating and drying with a dehydrator-dryer.

A feed slurry was prepared by adding a low-concentration nickel sulfate aqueous solution to the deleaded starch obtained from the deleading step of the nickel hydrometallurgical process to form a slurry. Next, the slurry concentration of the supply slurry was adjusted to 250 to 400 g / L to prepare test materials (concentration adjustment slurry) according to Examples and Comparative Examples, and a sulfuric acid dissolution operation was performed.
The chemical composition of the solid component in the supply slurry is 45 to 55% by weight of Ni, 1 to 5% by weight of Co, 0.01 to 0.05% by weight of Fe, and 0.1 to 0.5% by weight of Cu. % And Cl was 5 to 7% by weight. This chemical component analysis was performed with a fluorescent X-ray analyzer.

The sulfuric acid dissolution operation is performed in a batch processing step. Specifically, the supply slurry (concentration adjustment slurry) shown in Table 1 adjusted to a slurry concentration of 250 to 400 g / L is received in the dissolution tank, and the slurry temperature is set to 95 ° C. Example 1 prepared by adding a 70% by weight sulfuric acid aqueous solution to the slurry so that the liquid temperature was maintained at 95 ° C. and the pH was maintained in the range of 1.4 to 1.6. 2 and Comparative Example 1 were obtained.
The produced dissolved solution chlorine concentration was measured and displayed in FIG.
As a result, in both Example 1 (corresponding to the invention of claim 1) and Example 2 (corresponding to the invention of claim 2), the chlorine concentration of the solution was in the range of 140 to 160 mg / L.

From FIG. 2, the solution chlorine concentration shows a sharp decrease until the slurry concentration of the feed slurry reaches around 360 g / L, but when the slurry concentration is about 350 to 360 g / L, the solution chlorine concentration is the lowest. When the slurry concentration was lower than 360 g / L, no decrease in the solution chlorine concentration value was observed, and a tendency to increase slightly was also observed.
If the concentration is less than 300 g / L, the chlorine concentration of the solution can be almost the same as the minimum value, but the nickel concentration of the solution is lowered, so the efficiency is lowered in the subsequent step of removing impurities in the solution. However, the processing cost increases, and in the concentration and crystallization process of the high-purity nickel sulfate aqueous solution, there is a possibility that the energy consumption for the concentration increases and the processing cost increases. In addition, for use within that range, it is desirable to consider the occurrence of the above problems.
Therefore, the preferable slurry concentration of the slurry supplied to the sulfuric acid dissolution operation is 360 g / L or less (Example 1), more preferably 300 g / L or more and 360 g / L or less (Example 2).

Claims (3)

A mixture comprising at least chlorine, nickel hydroxide, and cobalt hydroxide,
The mixture comprises 5-10 wt% chlorine, 35-60 wt% nickel, and 1-10 wt% cobalt ;
After adding a slurry aqueous solution to the mixture to form a concentration adjustment slurry having a slurry concentration of 360 g / L or less, a solution for dissolving the solid component of the slurry prepared by adding sulfuric acid to the concentration adjustment slurry, By maintaining the temperature of the solution at 60 ° C. or higher and controlling the pH of the solution to 2.0 or less to dissolve the solid component of the concentration-adjusted slurry and remove chlorine contained in the slurry. A method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate, characterized in that a mixed aqueous solution of nickel sulfate and cobalt sulfate having a low chlorine concentration is obtained.   The method for producing a low chlorine concentration mixed aqueous solution of nickel sulfate and cobalt sulfate according to claim 1, wherein the concentration adjusting slurry has a slurry concentration of 300 to 360 g / L.   The low chlorine concentration of nickel sulfate and cobalt sulfate according to claim 1 or 2, wherein the solid component of the concentration adjusting slurry is dissolved by controlling the pH of the solution to be maintained at 1.5 or less. A method for producing a mixed aqueous solution.