KR20180073895A - Method for recovering carbonate from slag and system therefor - Google Patents

Abstract

The present invention relates to a method for treating steel slag, in which carbonates are extracted from the steel slag and reused as carbonates, the steel slag is recycled and CO_2 gas can be utilized without being released into the atmosphere, to a method for recovering the carbonates by using the steel slag which can be reused by recovering remaining ligand after completion of a reaction in a system and to the system therefor.

Description

[0001] METHOD FOR RECOVERING CARBONATE FROM SLAG AND SYSTEM THEREFOR [0002]

More particularly, the present invention relates to a method and a system for extracting metal ions contained in steelmaking slag and recovering extracted metal ions as carbonates.

Slag is a product that necessarily occurs in a steel smelting process. Slag is inevitably produced by gangue components of iron ore or coke in the steelmaking process, oxides generated in the oxidation and deoxidation of molten iron or molten steel in the steelmaking process, or additives added for refining purposes.

In the steelworks, the amount of blast furnace slag and steel slag generated as an industrial by-product each year is rapidly increasing, but due to the lack of efforts to develop and apply these byproducts compared to the amount generated, most of them are buried or left in the site Environmental problems are becoming serious.

The slag is composed of SiO ₂ and CaO, and contains Al ₂ O ₃ , FeO, MgO, P ₂ O 5 and CaS depending on the type of refining reaction. The steelmaking slag based on the oxidation reaction of molten iron or molten steel is based on CaO-SiO ₂ -FeO.

Various techniques for utilizing such steelmaking slag have been developed. As disclosed in Korean Patent No. 10-1487977, a method of recovering Fe in steelmaking slag and a method of recovering Fe in slag as in Korean Patent No. 10-1175422 However, this is about the recovery of the Fe component in the steelmaking slag, and a technology capable of recovering other components has not been developed.

Accordingly, it is urgent to develop a technique for recovering metal components that can be extracted from steelmaking slag.

The present invention relates to a method for recovering carbonate using steelmaking slag and a system thereof.

The present invention provides a method and a system for recovering carbonate by using steelmaking slag capable of recycling steel-making slag and utilizing CO ₂ gas, by extracting metal ions of steel-making slag and recovering it as carbonate by reacting with carbon dioxide .

Another object of the present invention is to provide a method and a system for recovering carbonate by using steelmaking slag capable of recovering and reusing a regenerated ligand after the production of carbonate mineral in steelmaking slag.

Other objects and advantages of the present invention will become more apparent from the following detailed description of the invention and claims.

The embodiments of the present invention are described in order to more fully explain the present invention to those skilled in the art, and the following embodiments may be modified into various other forms, It is not limited to the embodiment. Rather, these embodiments are provided so that this disclosure will be more faithful and complete, and will fully convey the scope of the invention to those skilled in the art.

In the drawings, the thickness and the size of each layer are assumed for convenience and clarity of description, and the same reference numerals denote the same elements in the drawings. As used herein, the term "and / or" includes any and all combinations of one or more of the listed items.

The terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. As used herein, the singular forms "a," "an," and "the" include singular forms unless the context clearly dictates otherwise. Also, " comprise "and / or" comprising "when used herein should be interpreted as specifying the presence of stated shapes, numbers, steps, operations, elements, elements, and / And does not preclude the presence or addition of one or more other features, integers, operations, elements, elements, and / or groups.

In one embodiment of the present invention, the present invention provides a method for producing a mixture comprising: 1) mixing a steelmaking slag and an acidic solvent to prepare a mixture comprising metal ions; 2) passing the first mixture of step 1) through a first filter to separate into a second mixture comprising metal ions and a residue; 3) adding a ligand to the second mixture of step 2) and mixing to prepare a third mixture comprising a complex prepared by reacting a metal ion with a ligand; 4) separating the complex by the electrochemical method of the third mixture in the step 3); 5) reacting the complex in step 4) with carbon dioxide to produce a carbonate; And 6) separating the carbonates produced in step 5). The present invention also relates to a method for recovering carbonates using steel slag.

According to an embodiment of the present invention, in the step 6) of the present invention, the mixed solution in which the carbonate formation reaction has been completed in the step 5) is passed through a filter including micro-sized pores to recover the carbonate which has not passed through the filter have.

In one embodiment of the present invention, the filter of step 6) of the present invention has a pore diameter of 30 to 40 mu m, but is not limited to the examples.

In one embodiment of the present invention, the mixed solution having passed through the filter of the present invention may be recovered and supplied to a reaction vessel for producing the third mixture of step 3).

In one embodiment of the invention, 1) an acidic solvent of the steps of the present invention is nitric acid (HNO _3), hydrochloric acid (HCl), sulfuric acid (H ₂ SO _4), bromide acid (HBr), iodine hydrofluoric acid (HI ), Perchloric acid (HClO ₄ ), and phosphoric acid (H ₃ PO ₄ ), but the present invention is not limited to these examples.

In one embodiment of the present invention, the metal ion of step 1) of the present invention is Ca ^{2 +,} but is not limited to the examples.

In one embodiment of the present invention, CH ₃ COOH, C ₆ H ₉ NO ₆ , C ₆ H ₅ NO ₂ , HN (CH ₂ CO ₂ H) ₂ , Citrate ³⁺ (Citrate ³ + ), Glutamate ⁺ (glutamate ⁺ ), and C ₂ H ₂ O ₄ , but the present invention is not limited to these examples.

In one embodiment of the present invention, the carbonate of the present invention is CaCO _3, but the present invention is not limited thereto.

In one embodiment of the present invention, the first filter of the present invention may include pores having a diameter of 30 to 50 占 퐉, but the present invention is not limited to the examples.

According to one embodiment of the present invention, the present invention provides a method of producing a steel slag, comprising: a metal ion extracting unit for mixing a steelmaking slag and an acidic solvent to produce a first mixture containing metal ions; A separator for separating the first mixture produced in the metal ion extractor into a second mixture and a residue comprising metal ions; A complex compound production unit for adding a ligand to the second mixture separated from the first separation unit and mixing the metal ion and the ligand to produce a complex; A complex-compound separating unit for separating a complex produced by the complex-compound-producing unit; A carbonation unit for producing carbonates by reacting the complex compound separated in the complex separation unit with carbon dioxide; And a carbonate separator for separating carbonates produced in the carbonated hollow section. The present invention also relates to a system for recovering carbonates using steelmaking slag.

In one embodiment of the present invention, the carbonate separation unit of the present invention can recover the carbonate which has not passed through the filter by passing the mixed solution in which the carbonation reaction has been completed in the carbonation purification unit through a filter including micro-sized pores .

In one embodiment of the present invention, the carbonate separation unit of the present invention may further include a recovery unit for recovering the carbonate and transferring the remaining mixture solution to the complex compound supply unit.

The present invention relates to a method and a system for recovering carbonates using steelmaking slag, which can extract carbonates from steelmaking slag and use carbonates, recycle steelmaking slag, and utilize CO ₂ gas without releasing it to the atmosphere , The method of treating steelmaking slag, and the ligand used in the system can be recovered and reused.

1 is a flowchart illustrating a method for recovering carbonate using steelmaking slag according to an embodiment of the present invention.
2 is a system for recovering carbonate using steelmaking slag according to an embodiment of the present invention.
3 is a system for recovering carbonate using steelmaking slag according to an embodiment of the present invention.
4 is a conceptual diagram of a single-vessel desalination apparatus according to an embodiment of the present invention.
100: Metal ion extraction unit
200:
300:
400: Complex separation unit
500: Carbonation core
600: carbonate separator
700:
910: Cathode carbon fiber electrode
920: anode carbon fiber electrode
930: Cation exchange membrane
940: Anion exchange membrane

A method and system for recovering a carbonate using the steel making slag of the present invention will be described with reference to the drawings.

FIG. 1 is a flowchart illustrating a method of recovering carbonate using steelmaking slag according to an embodiment of the present invention. Referring to FIG. 1, a step (S100) of preparing a first mixture by mixing a steelmaking slag and an acidic solvent; 2) separating the first mixture of step 1) into a second mixture and a residue (step S200); 3) adding a ligand to the second mixture of step 2) and mixing to prepare a third mixture (S300); 4) separating the complex contained in the third mixture of step 3) (S400); 5) reacting the separated complex with CO ₂ ; And 6) separating the formed carbonate by reacting with CO ₂ (S500). Hereinafter, the method of recovering the carbonate will be described step by step.

The step 1) is a step (S100) of mixing a steelmaking slag and an acidic solvent to produce a first mixture (S100). More specifically, to facilitate the reaction with the acidic solvent by recovering the steelmaking slag, a jaw crusher , And the particles having a diameter of less than 1000 탆 are sieved using a sieve. In other words, if the particle size is reduced, the steel sheet can be finely divided into a primary crushing operation and a secondary crushing operation in order to increase the contact area with the acidic solvent. Steelmaking slag having a fine particle size is mixed with an acidic solvent and allowed to react. Wherein the acidic solvent is nitric acid (HNO _3), hydrochloric acid (HCl), sulfuric acid (H ₂ SO _4), bromide acid (HBr), iodine hydrofluoric acid (HI), perchloric acid (HClO ₄₎ and phosphoric acid (H ₃ PO ₄ ), And preferably a nitric acid (HNO ₃ ) solvent of 1.0, 1.5, and 2.5 M, but is not limited to the examples. When the steelmaking slag and the acidic solvent are mixed, the metal components in the steelmaking slag are present in the form of metal ions in the acidic solvent. Therefore, the first mixture is present in a mixed state of the steelmaking slag, the acidic solvent, and the metal ion. In order to allow the metal component of the steelmaking slag to react with the acidic solvent to exist as a metal ion, stirring can be performed using a magnetic bar.

The step 2) is a step (S200) of separating the first mixture of step 1) into a second mixture and a residue (S200). More specifically, the first mixture is a mixture of steel making slag, acidic solvent, , Which is passed through a filter to pass only the acidic solvent and the metal ion, and the components such as unreacted steelmaking slag can be classified as residues. In the case of the first mixture, steel-making slag and an acidic solvent are reacted to extract metal ions, but steel-making slag that does not react with an acidic solvent and components other than metal components are mixed. . The first filter includes pores having a diameter of 30 to 50 占 퐉, and the components other than the large unreacted steel making slag and the metallic component can not be passed through the first filter and can be classified into a residue. The second mixture may include a metal ion and an acidic solvent because the particle size of the acidic solvent and the metal ion component pass through the first filter.

The third step is a step (S300) of adding a ligand to the second mixture of step 2) and mixing to prepare a third mixture. More specifically, the ligand is put into a second mixture containing a metal ion and an acidic solvent, The ligand can be reacted with metal ions by mixing to form a complex. The ligand means a molecule or ion bonded around the central metal ion of a coordinating compound and is characterized in that it has a pair of unshared electrons in order to coordinate bond with the metal ion. The ligand selectively reacts with the metal ion. Therefore, the calcium ion (Ca ²⁺ ) can be selectively extracted from the various metal ions of the second mixture. That is, the metal ions can be selectively extracted by using the property that the ligand binds to a specific metal ion. The ligand is _{CH 3 COOH, C 6 H 9} NO 6, C 6 H 5 NO 2, HN (CH 2 CO 2 H) 2, citrate ^{3 +} (Citrate ^{3 +),} glutamate ⁺ (glutamate ⁺⁾ and C ₂ H ₂ O ₄ , preferably C ₂ H ₂ O _4, but any ligands capable of selectively coordinating to the calcium ion (Ca ^{2 +} ) can be used, It is not. Thus, the third mixture may comprise an acidic solvent, complex compound, unreacted ligand and unreacted metal ion.

The step 4) is a step (S400) of separating the complex compound contained in the third mixture of step 3), more specifically, the step of separating the complex compound from the third mixture containing the acidic solvent, complex compound, unreacted ligand and unreacted metal ion . ≪ / RTI > The coordination complex can be separated by the electrochemical method using the property of not charging. The electrochemical method can be separated into metal ions unreacted with the complex compound and the ligand by using a storage-type desalination device. The unreacted metal ion is, for example, Fe ^{2 +} , Si ²⁺ or Al ^2+, but metal ions other than the exemplified metal ions may be included depending on the steel making slag, and are not limited to the examples. The storage desalination apparatus includes a pair of electrodes; A pair of carbon fiber electrodes; And a pair of ion exchange membranes, wherein the pair of electrodes are disposed at both ends, a pair of carbon fiber electrodes are formed on the inner surfaces of the pair of electrodes, and the inner side of the pair of carbon fiber electrodes A pair of ion exchange membranes can be formed.

The separation by electrochemical method utilizes the property that the ligand has a negative charge and the unreacted metal ion has a positive charge. When the third mixture in the step 3) is passed through a condensate desalination device, a ligand having a negative charge moves toward the positive electrode of the storage and desalination device, unreacted metal ions having a positive charge move toward the negative electrode, Through an ion exchange membrane which can selectively pass the ion exchange membrane. The ion exchange membrane not only maximizes the adsorption efficiency at each electrode, but also facilitates the recovery of the desorbed ions when the ions are desorbed.

What is classified by the electrochemical method is an acidic solvent and a complex compound, and through the step of reacting CO ₂ with the classified complex (S500), a carbonate can be formed. Reaction of the complex with CO ₂ will be referred to as carbonation process. That is, when the complex classified by the electrochemical method is reacted with CO ₂ , the metal ion (Ca ^{2 +} ) of the complex in which the ligand is coordinated around the metal ion is more reactive with CO ₂ than the ligand, ₂ to form a carbonate, and the ligand breaks the coordination bond and is present in the solution. That is, the carbonates can be produced by utilizing high reactivity between metal ions and CO ₂ . However, in this carbonation process, the solution should be basicized to increase the reactivity between metal ions and CO ₂ . 4) Since the solution classified in step S400 is a mixture of an acidic solvent and a complex, the solution will be said to be acidic. When the solution is acidic, even if CO ₂ is added, the reactivity of the carbonate is deteriorated. To avoid this problem, 4) Strong base is added to the solution classified in step S400 and mixed to make the solution exhibit basicity. 4) The pH of the solution classified in step S400 is about 2, but a base is added to increase the pH to about 9, and the base to be added is a strong base such as NH ₄ OH, NaOH or KOH, If the pH of the solution can be increased, it is not limited to the base type in the above example, but can be used.

As described above, the carbonates prepared using the high reactivity of metal ions (Ca ^{2 +} ) and CO ₂ can be recovered only through the separation step S 600. The carbonate is CaCO ₃ , and is passed through a second filter to obtain only carbonate. And the second filter includes a plurality of pores having a diameter of 30 to 40 mu m. When the solution is passed through the second filter after the carbonation process because the size of the carbonate is larger than 40 mu m, the carbonate that has not passed through the second filter remains, and the carbonate that remains in the solution after passing through the second filter is not left.

Solution that has passed through the second filter, the carbonate does not exist, there is carbon dioxide and the unreacted complex of the metal ion (Ca ^{+ 2)} and a separate ligand. Thus, the solution having passed through the second filter is recovered separately and is transferred to the reactor for producing the third mixture in the step 3). In order to produce the third mixture in the step 3), the need to purchase a ligand is reduced, and the ligand used in the carbonate recovery method can be reused, so that resources can be recycled and the cost reduction effect I will say it is excellent. Further, a solution for recovery and recycling has a complex compound. By reacting the complex again with CO ₂ , the recovery rate of the carbonate can be improved.

2 and 3 relate to a system for recovering carbonate using steelmaking slag according to an embodiment of the present invention.

2, the system for recovering carbonate using steelmaking slag according to an embodiment of the present invention includes a metal ion extraction unit 100, a separation unit 200, a complex compound production unit 300, a complex compound separation unit 400, And may include a carbonation unit 500 and a carbonate separation unit 600.

More specifically, the metal ion extraction unit 100 relates to mixing a steelmaking slag and an acidic solvent to produce a first mixture containing metal ions. A method for producing a first mixture, which comprises reacting a metal component contained in a steelmaking slag with a metal ion, reacting the metal component with an acidic solvent to extract a metal ion, mixing a steelmaking slag with an acidic solvent to prepare a first mixture, Unreacted steel making slag, acidic solvent and metal ion.

The separation unit 200 separates the first mixture generated in the metal ion extraction unit 100 into a second mixture and a residue containing metal ions, and the first mixture is an unreacted Steelmaking slag, acidic solvent and metal ion. Therefore, unnecessary unreacted steel making slag in the carbonate recovery system of the present invention can be sorted and recovered as a residue to obtain a second mixture containing an acidic solvent and a metal ion.

The complex-compound-producing unit 300 is prepared by adding a ligand to a second mixture separated from the separating unit 200, and mixing the metal ions with the ligand to produce a complex. The ligand, as mentioned above, can coordinate with a specific metal ion to form a complex. That is, among the plurality of metal ions contained in the second mixture, a ligand capable of selectively reacting only calcium ions (Ca ²⁺ ) to form a complex is included in the second mixture, and calcium ions Ca ²⁺ ) to form a complex.

The complex-compound separating unit 400 separates the complex compound produced in the complex-compound-producing unit 300, and more specifically, separates the complex compound and the ligand into metal ions unreacted with the depolymerization apparatus. The complex separation unit 400 can efficiently separate only the complex using the property that the complex is not charged and the ligand and the unreacted metal ion are charged.

The carbonated crystal unit 500 reacts the complex compound separated in the complex compound separation unit 400 with carbon dioxide to produce carbonate. The ligand selectively reacts with the metal ion to form a complex. When the complex is reacted with CO ₂ , the metal ion (Ca ^{2 +} ) of the complex is highly reactive with CO ₂ than the ligand. When the carbon dioxide is encountered, Carbonates can be prepared using the property of reacting with CO ₂ to form a carbonate. However, even if CO ₂ is reacted in the case of a solution having an acidity, the solution flowing into the carbonation unit 500 is acidic, and a buffer for increasing the pH of the acid solution Buffer solution, and the buffer solution may use a strong base such as NH ₄ OH, NaOH or KOH, but is not limited to the examples.

The carbonate separator 600 separates carbonates produced in the carbonation purification unit 500 and includes a filter including a plurality of pores having a diameter of 30 to 40 μm. Since the diameter of the pores in the filter of the carbonate separator 600 is at most 40 占 퐉, the carbonate having a diameter exceeding 40 占 퐉 can not pass through the carbonate separator 600, Only the carbonate can be separated.

FIG. 3 shows another embodiment of the present invention, and may further include a recovery unit 700. The recovering unit 700 recovers the mixed solution that has passed through the carbonate separating unit 600 and transfers the recovered mixed solution to the complexing material producing unit 300. The carbonate separating unit 600 separates The recovering unit 700 may further include a recovery unit 700 for recovering the mixed solution that has passed through the filter, through which the mixed solution is passed through a filter including micro-sized pores, and the carbonate that has not passed through the filter is recovered . The mixed solution having passed through the filter recovered in the recovery unit 700 has a complex compound not reacting with carbon dioxide and a ligand separated from the metal ion (Ca ²⁺ ), and is recovered through the recovery unit 700, By moving to the complex-compound-producing section 300, the need to purchase a ligand to produce a complex compound is reduced, and the ligand used in the carbonate recovery method can be reused, making it possible to recycle resources and reduce costs The effect of Further, a solution for recovery and recycling has a complex compound. By reacting the complex again with CO ₂ , the recovery rate of the carbonate can be improved.

FIG. 4 is a conceptual view of a capacitative desalination apparatus according to an embodiment of the present invention, in which a pair of electrodes is composed of an anode and a cathode. When the complex compound, the unreacted ligand and the unreacted metal ion formed in the complex-compound-forming unit 300 pass through the charge-coupled desalination apparatus, the unreacted ligand and the unreacted metal ion are released to bind to the electrode of the charge- , And the unconjugated complex is allowed to pass through the depolarization apparatus. When the solvent containing the complex compound passes through the electrolytic desalination device, the potential of the electrode of the charge and discharge desalination device is adjusted to desorb and recover the adsorbed unreacted ligand and unreacted metal ion, and then returned to the metal ion extracting section 100 And transport it.

4, a carbon fiber electrode 910 as a cathode, a carbon fiber electrode 920 as an anode, a cation exchange membrane 930, an anion exchange membrane 940, and a pair of electrodes (not shown) ). The pair of electrodes are disposed at both ends, a pair of carbon fiber electrodes 910 and 920 are formed on the inner surfaces of the pair of electrodes, and the inner side of the pair of carbon fiber electrodes 910 and 920 A pair of ion exchange membranes 930 and 940 may be formed.

The carbon fiber is excellent in heat resistance, impact resistance, and resistance to chemicals. In the heating process for the production of carbon fiber, molecules such as oxygen, hydrogen, and nitrogen escape, and the weight is lighter, and the elasticity and strength are excellent. In addition, it has a high electrical conductivity, a large elastic modulus, flexibility, and thus has a large bending deformation capacity, so that it can be easily formed into various patterns and shapes.

The pair of carbon fiber electrodes 910 and 920 may be formed to surround a pair of coating layers (not shown), and the pair of coating layers (not shown) may be formed of a porous carbon material, Active carbon slurry, graphene, CNT and the like can be selected.

The carbon fiber electrodes 910 and 920 have a self-ion-adsorbing ability due to porosity and are superior in adsorption ability than activated carbon. In addition, the pair of electrodes (not shown) include a pair of coating layers (not shown) together with a pair of carbon fiber electrodes 910 and 920 to form a double adsorption structure, have.

The pair of ion exchange membranes 930 and 940 are formed inside the pair of carbon fiber electrodes 910 and 920, respectively, and selectively pass the ions to increase ion removal capability. The pair of ion exchange membranes 930 and 940 may be composed of an anion exchange membrane selectively passing anions and a cation exchange membrane selectively passing cations. The anion exchange membrane is formed on the anode side and the cation exchange membrane is formed on the anode side . This not only maximizes the adsorption efficiency at each electrode, but also allows ions desorbed at the time of ion desorption to be quickly discharged by the ion exchange membrane and the flow rate.

The pair of electrodes 910 and 920 can be fabricated by changing the thickness of the electrode according to the application and needs of the user.

Claims (12)

1) mixing a steelmaking slag and an acidic solvent to prepare a mixture containing metal ions;
2) passing the first mixture of step 1) through a first filter to separate into a second mixture comprising metal ions and a residue;
3) adding a ligand to the second mixture of step 2) and mixing to prepare a third mixture comprising a complex prepared by reacting a metal ion with a ligand;
4) separating the complex by the electrochemical method of the third mixture in the step 3);
5) reacting the complex in step 4) with carbon dioxide to produce a carbonate; And
6) A method for recovering a carbonate using a steelmaking slag, comprising the step of separating the carbonate produced in the step 5). The method according to claim 1,
In the step 6), the mixed solution having undergone the carbonate formation reaction in the step 5) is passed through a filter including micro-sized pores,
And recovering the carbonate which has not passed through the filter. 3. The method of claim 2,
Wherein the pore diameter is 30 to 40 占 퐉. 3. The method of claim 2,
And recovering the mixed solution having passed through the filter and supplying the mixed solution to the reaction vessel for producing the third mixture in step 3). The method according to claim 1,
The acidic solvent in step 1) may be at least one selected from the group consisting of nitric acid (HNO ₃ ), hydrochloric acid (HCl), sulfuric acid (H ₂ SO ₄ ), hydrobromic acid (HBr), hydroiodic acid (HI), perchloric acid (HClO ₄ ) H ₃ PO ₄ ). The method for recovering carbonate by using the steelmaking slag according to claim 1, The method according to claim 1,
Wherein 1) the metal ions of step is a method for recovering the carbonate using the steel-making slag Ca ^{+ 2.} The method according to claim 1,
The following steps: 1) the ligand is _{CH 3 COOH, C 6 H 9} NO 6, C 6 H 5 NO 2, HN (CH 2 CO 2 H) 2, citrate ^{3 +} (Citrate ^{3 +),} glutamate ⁺ (glutamate ⁺ ) And C ₂ H ₂ O ₄ , in which the carbonate slag is used. The method according to claim 1,
Wherein the carbonate is CaCO ₃ , and recovering the carbonate using the steel making slag. The method according to claim 1,
Wherein the first filter comprises pores having a diameter of 30 to 50 占 퐉. A metal ion extraction unit for mixing a steelmaking slag and an acidic solvent to produce a first mixture containing metal ions;
A separator for separating the first mixture produced in the metal ion extractor into a second mixture and a residue comprising metal ions;
A complex compound production unit for adding a ligand to the second mixture separated from the first separation unit and mixing the metal ion and the ligand to produce a complex;
A complex-compound separating unit for separating a complex produced by the complex-compound-producing unit;
A carbonation unit for producing carbonates by reacting the complex compound separated in the complex separation unit with carbon dioxide; And
And a carbonate separator for separating carbonates produced in the carbonated coagulation unit. 11. The method of claim 10,
The carbonate separator may be configured such that the carbonic acid-generating mixed solution is passed through a filter including micro-sized pores,
And recovering the carbonate which has not passed through the filter. 11. The method of claim 10,
Wherein the carbonate separation section further comprises a recovery section for recovering the carbonate and transferring the remaining mixed solution to the complex compound supply section.

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