Manufacturing method of battery material

Abstract

The purpose of the present disclosure is to provide a method for producing a battery material that improves the recovery rate of valuable metals. The method for manufacturing a battery material disclosed herein includes: a preparation step of preparing a recovery target containing at least one of Ni and Co; an acid exudation step in which the object to be recovered is immersed in an acid solution to obtain an acid exudate; a neutralization and precipitation step in which the acid exudate is mixed with a neutralizer to obtain a precipitate; a solid-liquid separation step in which the precipitate is subjected to solid-liquid separation; and an ammonia exudation step in which the separated precipitate is immersed in an ammonia solution containing ammonium ions to obtain an ammonia exudate containing at least one of Ni and Co.

Description

Technical Field

[0001] The technology disclosed herein relates to a method for producing battery materials. Background Art

[0002] Lithium-ion secondary batteries are widely used in various fields. The lithium-ion secondary batteries use various materials including valuable metals such as Ni and Co. For example, lithium transition metal composite oxides such as lithium nickel composite oxide, lithium cobalt composite oxide, lithium nickel cobalt composite oxide, and lithium nickel cobalt manganese composite oxide are used as positive electrode active materials. In addition, aluminum and the like are used as positive electrode cores.

[0003] In recent years, recycling technology is being developed to recover valuable metals from used batteries, engineering end materials, etc. and reuse them as battery materials. For example, Japanese Patent Publication No. 2020-164971 discloses an example of a recycling technology for positive plates. In the recycling method described in Japanese Patent Publication No. 2020-164971, the recovery object (lithium-ion battery waste) is leached with acid, and the leached liquid obtained by the above leaching is neutralized, thereby removing at least a part of the aluminum ions from the leached liquid to obtain a neutralized liquid, and the above neutralized liquid is subjected to solvent extraction, thereby extracting the remaining part of the aluminum ions from the neutralized liquid. It is disclosed that cobalt (Co) and / or nickel (Ni) can be recovered from the extraction residual liquid from which aluminum has been removed.

[0004] Prior art literature

[0005] Patent Literature

[0006] Patent Document 1: Japanese Patent Publication No. 2020-164971 Summary of the invention

[0007] As disclosed in the above-mentioned Japanese Patent Publication No. 2020-164971, in the previous positive plate recovery technology, at least a portion of the aluminum ions (aluminum) are precipitated and removed in the form of a precipitate by neutralizing the acid exudate containing the recovery object. However, a portion of the precipitate may contain valuable metals (Ni and / or Co). Therefore, in the previous positive plate recovery technology, it is possible to remove the valuable metal from the recovery object and fail to fully recover the valuable metal.

[0008] The present disclosure has been made in view of the above circumstances, and an object of the present disclosure is to provide a method for producing a battery material with an improved recovery rate of valuable metals.

[0009] In order to solve the above-mentioned problems, a method for producing a battery material having the following structure (hereinafter also simply referred to as a “production method”) is provided.

[0010] The manufacturing method of the battery material disclosed herein includes: a preparation step of preparing a recovery object containing at least one of Ni and Co; an acid leaching step of immersing the above-mentioned recovery object in an acid solution to obtain an acid leaching solution; a neutralization precipitation step of mixing the above-mentioned acid leaching solution with a neutralizer to obtain a precipitate; a solid-liquid separation step of performing solid-liquid separation on the above-mentioned precipitate; and an ammonia leaching step of immersing the above-mentioned separated precipitate in an ammonia solution containing ammonium ions to obtain an ammonia leaching solution containing at least one of the above-mentioned Ni and the above-mentioned Co.

[0011] In the manufacturing method of the above configuration, by subjecting the precipitate obtained in the neutralization precipitation step to ammonia seepage, Ni and / or Co in the precipitate can be separated and dissolved in an ammonia solution. This can improve the recovery rate of valuable metals from the recovery target. BRIEF DESCRIPTION OF THE DRAWINGS

[0012] Figure 1 It is a longitudinal cross-sectional view schematically showing the internal structure of a lithium-ion secondary battery.

[0013] Figure 2 It is schematically indicated Figure 1 A perspective view of an electrode body of a lithium-ion secondary battery shown.

[0014] Figure 3 This is a flowchart illustrating a method for producing a battery material according to one embodiment.

[0015] Figure 4 It is a detailed description Figure 3 Flowchart of the solvent extraction process. DETAILED DESCRIPTION

[0016] Hereinafter, the implementation methods of the technology disclosed herein will be described with reference to the accompanying drawings. It should be noted that matters other than those specifically mentioned in this specification and matters required for implementing the technology disclosed herein can be grasped as design matters based on the prior art in the field by those skilled in the art. The technology disclosed herein can be implemented based on the contents disclosed in this specification and the technical common sense in the field. In addition, the expression "A to B" indicating a range in this specification includes the meaning of above A and below B, and also includes the meaning of "preferably greater than A" and "preferably less than B".

[0017] 1. Recycling objects

[0018] The manufacturing method of the battery material of the present embodiment manufactures the battery material (typically the material of the positive electrode active material of the lithium ion secondary battery, the precursor of the positive electrode active material, the positive electrode active material) by recovering valuable metals such as Ni and Co from the specified recycling object. As an example of the recycling object here, a used lithium ion secondary battery can be cited. The lithium ion secondary battery is described in detail below. Figure 1 It is a longitudinal cross-sectional view schematically showing the internal structure of a lithium-ion secondary battery. Figure 2 It is schematically indicated Figure 1 A perspective view of an electrode body of a lithium-ion secondary battery shown.

[0019] like Figure 1 As shown, the lithium ion secondary battery 1 includes a case 10 , an electrode body 20 , and an electrolyte (not shown).

[0020] (1) Housing

[0021] The shell 10 is a box-shaped container. The inside of the shell 10 contains the electrode body 20 and the electrolyte. The shell 10 is made of a metal material with a certain strength (aluminum (Al) or the like). In addition, the shell 10 is equipped with a positive terminal 12 and a negative terminal 14. The positive terminal 12 and the negative terminal 14 are connected to the electrode body 20 inside the shell 10. Specifically, the positive terminal 12 is connected to the positive electrode plate 30 (see Figure 2 ) is connected. Aluminum (Al) or the like is used for the positive electrode terminal 12. On the other hand, the negative electrode terminal 14 is connected to the negative electrode plate 40 of the electrode body 20. Copper (Cu) or the like is used for the negative electrode terminal 14.

[0022] (2) Electrode body

[0023] The electrode body 20 is a power generation element of the lithium ion secondary battery 1. Figure 2 As shown, the electrode body 20 includes a positive electrode plate 30, a negative electrode plate 40 and a separator 50. Figure 2 The electrode body 20 shown is a wound electrode body. The wound electrode body is made by stacking a positive electrode plate 30, a negative electrode plate 40, and a separator 50 to form a long strip-shaped laminate, and winding the laminate. However, the structure of the electrode body 20 is not particularly limited, and may be other structures known in the past (laminated electrode body, etc.).

[0024] The positive electrode plate 30 includes a positive electrode core 32 as a conductive metal foil and a positive electrode active material layer 34 applied to the surface of the positive electrode core 32. The positive electrode core 32 uses aluminum (Al) or the like. In addition, the positive electrode active material layer 34 is a composite material layer containing a positive electrode active material, a conductive material, a binder, etc. The positive electrode active material is a lithium transition metal composite oxide containing at least one of nickel (Ni) and cobalt (Co). As an example of the lithium transition metal composite oxide, lithium nickel composite oxide, lithium cobalt composite oxide, lithium nickel manganese composite oxide, lithium manganese cobalt composite oxide, lithium nickel cobalt composite oxide, lithium nickel manganese cobalt composite oxide, etc. can be cited. According to the manufacturing method of this embodiment, Ni and / or Co can be efficiently recovered from the recycling object containing such a lithium transition metal composite oxide. In addition, as a conductive material, carbon materials such as acetylene black and graphite can be cited. In addition, as a binder, resin materials such as polyvinylidene fluoride (PVdF) can be cited.

[0025] On the other hand, the negative electrode plate 40 includes a negative electrode core 42 which is a conductive metal foil and a negative electrode active material layer 44 applied to the surface of the negative electrode core 42. Copper (Cu) or the like is used for the negative electrode core 42. In addition, the negative electrode active material layer 44 is a composite layer containing a negative electrode active material, a binder, a thickener, and the like. As an example of a negative electrode active material, carbon materials such as graphite, hard carbon, and soft carbon can be cited. In addition, as other examples of negative electrode active materials, lithium titanate (LTO), silicon carbide, a composite containing carbon and silicon, silicon oxide (SiO X ) etc. As the binder, there can be mentioned resin materials such as styrene butadiene rubber (SBR). As the thickener, there can be mentioned resin materials such as carboxymethyl cellulose (CMC).

[0026] In addition, the separator 50 is an insulating sheet between the positive electrode plate 30 and the negative electrode plate 40. The separator 50 uses, for example, a resin material such as polyethylene (PE), polypropylene (PP), polyester, cellulose, polyamide, etc. In addition, a heat-resistant layer containing an inorganic filler can be formed on the surface of the separator 50. Examples of the inorganic filler include inorganic oxides such as aluminum oxide, magnesium oxide, silicon oxide, and titanium oxide, nitrides such as aluminum nitride and silicon nitride, metal hydroxides such as calcium hydroxide, magnesium hydroxide, and aluminum hydroxide, and clay minerals such as mica, talc, boehmite, zeolite, apatite, and kaolin.

[0027] (3) Electrolytes

[0028] The electrolyte is present between the positive electrode plate 30 and the negative electrode plate 40. Thus, the charge carrier (Li ion) can be moved between the positive electrode plate 30 and the negative electrode plate 40. As an example of the electrolyte, a non-aqueous electrolyte, a gel electrolyte, etc. can be cited. It should be noted that the electrolyte can be used without particular limitation for an electrolyte that can be used in a lithium ion secondary battery, and is not limited to the technology disclosed herein.

[0029] As an example of a recycling object in the manufacturing method of the present embodiment, a lithium-ion secondary battery 1 is described above. However, the manufacturing method disclosed herein is not limited to a method in which the lithium-ion secondary battery 1 of the above-mentioned structure is used as a recycling object. For example, at the manufacturing site of a lithium-ion secondary battery, a portion of the positive plate is sometimes cut off when an electrode body is manufactured. The portion of the cut positive plate (engineering end material) may also contain Ni and Co, and therefore may become a recycling object of the manufacturing method disclosed herein. In addition, at the manufacturing site of a lithium-ion secondary battery, sometimes the electrode body after manufacture has some defects and cannot be used in products. Such an electrode body may also contain Ni and Co, and therefore may become a recycling object. That is, the recycling object of the manufacturing method disclosed herein only needs to contain at least one of Ni and Co as a valuable metal, and is not particularly limited to a specific structure.

[0030] 2. Manufacturing methods of battery materials

[0031] Hereinafter, a method for producing the battery material according to the present embodiment will be described. Figure 3 It is a flowchart explaining the manufacturing method of this embodiment. Figure 4 It is a detailed description Figure 3 Flowchart of the solvent extraction process.

[0032] like Figure 3 As shown, the manufacturing method of the battery material of this embodiment includes a preparation step S10, an acid seepage step S40, a neutralization precipitation step S50, a solid-liquid separation step S60, and an ammonia seepage step S70. The manufacturing method of the battery material disclosed herein may further include a roasting step S20, a sorting step S30, a solvent extraction step S80, a Li crystallization step S90, a precursor preparation step S100, and an active material generation step S110. In addition, the manufacturing method disclosed herein may further include other steps at any stage, and the manufacturing process other than these may be the same as before. Below, each step is described.

[0033] (1) Preparation step S10

[0034] In the preparation step S10, a recycling object including at least one of Ni and Co is prepared. As described above, the "recycling object" in the technology disclosed herein only needs to include at least one of Ni and Co. That is, the recycling object is not limited to the finished lithium-ion secondary battery, and includes engineering waste materials, defective parts (electrode bodies, etc.). It should be noted that since the details of the recycling object have been described, repeated descriptions are omitted.

[0035] (2) Calcination Step S20

[0036] In the roasting step S20, the recycling object is heated at a predetermined temperature. Thus, the liquid components (electrolyte, etc.) in the recycling object can be removed, and the resin components (adhesive, separator, etc.) can be carbonized. In addition, when the charged lithium-ion secondary battery 1 is used as the recycling object, the function as a battery can be stopped by implementing the roasting step S20. Thus, the subsequent steps can be safely implemented. For the method of the roasting step S20, the technology used in the previous recycling technology can be used without particular restrictions, and does not represent the technology disclosed herein, so the detailed description is omitted.

[0037] It should be noted that the roasting step S20 is not essential and can be omitted as needed. For example, sometimes the process end material for preparing the positive electrode plate 30 in the preparation step S10 does not need to remove the liquid component and does not need to stop the function as a battery. In this case, even if the roasting step S20 is omitted, the valuable metal can be efficiently recovered.

[0038] (3) Sorting process S30

[0039] In the sorting process S30, the various components contained in the recycling object are sorted. The method of the sorting process S30 can use a previously known method, for example, sorting can be performed using a sieve, visual inspection, etc. For example, in the case where the engineering end material of the positive electrode plate 30 is a recycling object, the positive electrode core 32 can be sorted from the engineering end material and removed from the recycling object. In addition, in the case where the electrode body 20 is a recycling object, in addition to the positive electrode core 32, the negative electrode plate 40 can also be removed from the recycling object. Furthermore, in the case where the lithium-ion secondary battery 1 is a recycling object, in addition to the above-mentioned positive electrode core 32 and negative electrode plate 40, the shell 10 can also be removed from the recycling object. As a result, the content of other metals (Al, Cu, etc.) in the recycling object is reduced, so it can help to improve the recovery efficiency of valuable metals (Co, Ni).

[0040] It should be noted that in the sorting step S30, the recycling object can be crushed as needed. This can improve the efficiency of sorting each component. For example, when the lithium-ion secondary battery 1 is the recycling object, the shell 10 and the electrode body 20 can be crushed. This makes it easy to remove the shell 10, the positive electrode core 32 and the negative electrode plate 40 from the recycling object.

[0041] In addition, the sorting step S30 is not intended to completely remove other metal components such as Al and Cu from the recycling object. The details will be described later. Even if other metal components remain in the recycling object, the valuable metals (Ni and / or Co) and other metal components can be fully separated in subsequent steps (such as the neutralization precipitation step S50 and the ammonia seepage step S70). That is, the sorting step S30 can also be appropriately omitted as needed. For example, in the case of a recycling object with a low content of other metal components (such as the engineering end material of the positive plate 30), even if the sorting step S30 is omitted, the valuable metals can be efficiently recovered.

[0042] (4) Acid seepage step S40

[0043] In the acid seepage step S40, the recovery object after the preparation step S10 (or the roasting step S20 or the sorting step S30) is immersed in an acid solution. As a result, the valuable metals (Ni and / or Co) in the recovery object are dissolved in the acid solution. It should be noted that in the acid seepage step S40, in addition to the valuable metals, other metal materials (Al, etc.) are sometimes dissolved in the acid solution. That is, the acid solution (hereinafter also referred to as "acid seepage solution") that has passed the acid seepage step S40 may contain, for example, Li, Al, Cu, Co, Ni, Mn, etc. It should be noted that the acid seepage step may adopt a conventionally known step without particular limitation. As an example, the pH of the acid solution used in the acid seepage step S40 is preferably -1.5 to 1.5 (more preferably -0.5 to 0.5). As a result, the metal components in the recovery object can be appropriately dissolved. It should be noted that as specific examples of acid solution, inorganic acids such as sulfuric acid, nitric acid, hydrochloric acid, phosphoric acid, and organic acids such as citric acid, ascorbic acid, oxalic acid, and acetic acid can be cited. In addition, in the acid seepage step S40, in addition to the acid solution, a reducing agent such as hydrogen peroxide can also be added. As a result, the dissolution rate of the recovery object in the acid solution can be increased, and the acid seepage step S40 can be shortened. In addition, in the acid seepage step S40, it is preferred to filter the acid seepage solution after the acid seepage. As a result, undissolved components (carbon components, etc.) can be effectively removed. It should be noted that the temperature of the acid solution is preferably above 50°C (more preferably above 55°C, particularly preferably above 60°C). As a result, the acid seepage step S40 can be shortened. In addition, the upper limit of the temperature of the acid solution is not particularly limited, and can be below 90°C, below 85°C, or below 80°C. The concentrations of Ni and Co (the sum of Ni and Co) in the acid seepage solution after the acid seepage step S40 are not particularly limited, but from the perspective of productivity, the higher the concentration, the more preferred. Therefore, the concentration of Ni and Co in the acid leaching solution (the sum of Ni and Co) is preferably 1.0 mol / L to 2.0 mol / L. The concentration of Ni and Co in the acid leaching solution (the sum of Ni and Co) can be determined by ICP analysis.

[0044] (5) Neutralization precipitation step S50

[0045] In the neutralization precipitation step S50, a neutralizing agent is added to the acid exudate obtained in the acid exudation step S40 to increase the pH of the acid exudate. As a result, the Al contained in the acid exudate is precipitated and precipitated in the form of hydroxide (Al(OH)3). As a result, a metal solution in which Al is almost removed from the acid exudate containing Li, Al, Cu, Co, Ni, Mn, etc. can be obtained. It should be noted that as a neutralizing agent used in the neutralization precipitation step S50, an alkaline solution with a pH of 11 to 15 (preferably pH 12 to 14) can be used. It should be noted that as specific examples of the neutralizing agent, sodium hydroxide aqueous solution, calcium hydroxide, etc. can be cited. Among them, as a neutralizing agent, it is preferred to include sodium hydroxide aqueous solution. The concentration of the neutralizing agent is not particularly limited, but from the viewpoint of productivity, the higher the concentration, the more preferred. Therefore, the concentration of the neutralizing agent is preferably 10 to 30wt%.

[0046] The pH adjusted in the neutralization precipitation step S50 is preferably pH 5.0 or above, preferably pH 5.1 or above, and more preferably pH 5.6 or above. When the pH of the acid exudate is low (typically less than pH 4.5), it is difficult for Al in the acid exudate to form a hydroxide. In other words, Al is difficult to separate from the acid exudate. As the pH of the acid exudate increases, the Al in the acid exudate can be precipitated and precipitated in the form of Al hydroxide. In other words, Al can be more appropriately separated from the acid exudate. On the other hand, there is no particular limitation on the pH adjusted in the neutralization precipitation step S50. As the pH increases, sometimes part of Ni and Co in the acid exudate also forms hydroxides and precipitates in the metal solution. Therefore, the pH adjusted in the neutralization precipitation step S50 is preferably pH 6.5 or below, and more preferably pH 6.2 or below. It should be noted that the details will be described later, and even if part of Ni and Co are precipitated, Ni and Co can be separated from the precipitate in the subsequent step (ammonia seepage step S70).

[0047] (6) Solid-Liquid Separation Step S60

[0048] In the solid-liquid separation step S60, the metal solution and the precipitate after the neutralization precipitation step S50 are subjected to solid-liquid separation. Thus, the precipitate and the metal solution containing the valuable metal (Ni and / or Co) and other metal components can be obtained respectively. The method of solid-liquid separation can use a conventionally known method, so a detailed description is omitted here. The metal solution obtained in the solid-liquid separation step S60 is not particularly limited thereto, but according to the metal components contained in the metal solution, by providing each recovery step (solvent extraction step S80) described later, the various metal components contained in the metal solution can be recovered.

[0049] As described above, in the neutralization precipitation step S50, Al in the acid leachate can be precipitated in the form of hydroxide. On the other hand, a part of Ni and / or Co also forms hydroxides, and these hydroxides can also be precipitated in the metal solution in the same way as the hydroxide of Al. That is, the precipitate obtained in the solid-liquid separation step S60 sometimes contains valuable metals (Ni and / or Co) in the form of hydroxides. In order to recover the valuable metals (Ni and / or Co) from the precipitate, for example, it can be considered to return the precipitate to the acid leachate obtained in the acid leachate step S40 and dissolve it. However, in this case, Al accumulates in the acid leachate (in other words, the Al concentration in the acid leachate increases), which leads to a decrease in the yield of the valuable metals (Ni and / or Co), so it is not preferred. Here, if Figure 3 As shown, the present embodiment is characterized in that, in addition to the neutralization precipitation step S50 and the solid-liquid separation step S60, an ammonia seepage step S70 is further provided. Thus, the recovery efficiency of valuable metals (Ni and / or Co) can be greatly improved. The following is a specific description.

[0050] (7) Ammonia Leakage Step S70

[0051] In the ammonia seepage step S70, the precipitate precipitated in the neutralization precipitation step S50 and obtained by solid-liquid separation in the solid-liquid separation step S60 is immersed in an ammonia solution. Thus, Ni and / or Co in the precipitate can be separated, and an ammonia solution (hereinafter referred to as "ammonia seepage solution") in which Ni and / or Co are dissolved can be obtained. In detail, the hydroxides of Ni and Co typically form ammine complexes in the ammonia solution. The ammine complexes are dissolved in the ammonia solution. On the other hand, Al (and Al hydroxide) does not form ammine complexes in the ammonia solution, and typically remains as a residue (precipitate) in the form of Al hydroxide (Al(OH)3). Thus, the valuable metals (Ni and / or Co) in the precipitate can be selectively recovered. It should be noted that the "ammonia solution" in this specification refers to an aqueous solution containing ammonium ions in water as a solvent.

[0052] Ammonia solution can be purchased as a commercial product (ammonia water), or a solution in which a solvent containing at least water and an ammonia salt are dissolved can be used. As the ammonia salt used in the ammonia solution, for example, ammonium hydroxide (NH4OH), ammonium sulfate ((NH4)2SO4), ammonium carbonate ((NH4)2CO3), ammonium bicarbonate (NH4HCO3), ammonium chloride (NH4Cl), ammonium fluoride (NH4F) and the like can be appropriately used. These compounds can be used alone or in combination of two or more.

[0053] In some preferred embodiments, the ammonia solution preferably contains at least one selected from ammonium sulfate, ammonium chloride, and ammonium acetate. They have a so-called role as a pH buffer material for the ammonia solution. In detail, the pH of the ammonia solution can be reduced. By reducing the pH of the ammonia solution, the dissolution of Al in the ammonia solution is suppressed, and Ni and Co appropriately form ammine complexes, thereby Ni and Co can be selectively and appropriately dissolved in the ammonia solution. Furthermore, according to the above-mentioned configuration, the ammonia concentration of the ammonia solution can be increased, so Ni and Co can appropriately form ammine complexes and appropriately dissolve in the ammonia solution. Therefore, Ni and Co in the precipitate can be selectively exuded (recovered) into the ammonia solution appropriately.

[0054] In the ammonia seepage step S70, the pH of the ammonia solution is preferably adjusted to pH 9.0 to 11.5 for ammonia seepage, and more preferably adjusted to pH 9.5 to 10.0. As the pH of the ammonia solution decreases, Ni and Co appropriately form ammine complexes, so these valuable metals (Ni and / or Co) can be appropriately recovered. In addition, when the pH is too high (typically exceeding pH 11.5), part of the Al in the precipitate forms a hydroxide complex ([Al(OH)4] ― ) and began to dissolve in the ammonia solution.

[0055] The ammonia concentration in the ammonia solution in the ammonia seepage step S70 is preferably 10 wt% or more, more preferably 20 wt% or more. As the ammonia concentration increases, Ni and / or Co appropriately form ammine complexes, so that valuable metals (Ni and / or Co) can be more efficiently recovered from the precipitate. On the other hand, from the viewpoint of the high volatility of ammonia, the upper limit of the ammonia concentration in the ammonia solution is not limited thereto, for example, 35 wt% or less, preferably 30 wt% or less.

[0056] It should be noted that the ammonium ions in the ammonia solution are used to form ammine complexes with Ni and / or Co. Therefore, as the ammonia seepage process proceeds, the pH and free ammonia concentration decrease compared to the initial ammonia solution (hereinafter also referred to as the "initial solution"). Therefore, additional ammonia solution can be added in the middle of the ammonia seepage process S70. Thereby, the pH and ammonia concentration in the ammonia solution can be maintained within a suitable range, and the separation of valuable metals (Ni and / or Co) in the precipitate can be performed more efficiently. The pH of the additional ammonia solution can be the same as that of the initial solution, or it can be higher. The ammonia concentration of the additional ammonia solution can be the same as that of the initial solution, or it can be higher. In addition, the composition of the additional ammonia solution can be the same as or different from that of the initial solution.

[0057] The temperature of the mixed solution in the ammonia seepage step S70 is not particularly limited, but is preferably 25° C. or higher, more preferably 40° C. or higher, and particularly preferably 60° C. or higher. Thus, the time of the ammonia seepage step S70 can be shortened. On the other hand, the upper limit of the temperature of the mixed solution is not particularly limited, but is preferably 100° C. or lower, more preferably 90° C. or lower, and particularly preferably 80° C. or lower.

[0058] It should be noted that the seepage time in the ammonia seepage process S70 may also vary according to, for example, the ammonia concentration in the reaction solution, the reaction temperature, etc., and is therefore not particularly limited, and is preferably approximately 0.5 hours or more, preferably 1 hour or more, and particularly preferably 2 hours or more. On the other hand, from the perspective of productivity, the seepage time is preferably approximately 8 hours or less, preferably 6 hours or less, and particularly preferably 4 hours or less. In addition, although not particularly limited, it is preferred to perform the ammonia seepage process S70 while stirring the ammonia solution. As a result, the contact area between the precipitate and the ammonia solution is increased, so that the valuable metals (Ni and / or Co) can be efficiently dissolved in the ammonia solution. Therefore, the seepage time can be shortened.

[0059] After the ammonia seepage step S70, the ammonia seepage liquid and the residue are subjected to solid-liquid separation. Thus, an ammonia seepage liquid in which Ni and / or Co are dissolved in an ammonia solution can be obtained. It should be noted that the use of the ammonia seepage liquid is not particularly limited thereto, and for example, it can be appropriately used as an alkaline solution in the precursor preparation step S100 described later. In this case, the ammonia seepage liquid can be directly used as an alkaline solution without going through steps such as washing. That is, there is no loss of valuable metals due to washing and re-extraction. In addition, the valuable metals (Ni and / or Co) in the ammonia seepage liquid can also be used as a precursor of a positive electrode active material. Therefore, the recovery rate of the valuable metals (Ni and / or Co) contained in the recovery object can be improved.

[0060] As described above, in the manufacturing method disclosed herein, by percolating the precipitate obtained in the neutralization precipitation step into an ammonia solution, the valuable metals (Ni and / or Co) in the precipitate can be recovered. Conventionally, the valuable metals (Ni and / or Co) are separated by performing a neutralization precipitation step on the acid permeate that has undergone the acid permeation step. At this time, a portion of the valuable metals (Ni and / or Co) will also precipitate together with Al as a precipitate, thereby causing a loss of the valuable metals, or there is a problem that in order to reduce the loss, the pH cannot be sufficiently increased in the neutralization precipitation step in order to suppress the precipitation of the valuable metals, and Al cannot be fully separated from the acid permeate. On the other hand, in the manufacturing method disclosed herein, the valuable metals (Ni and / or Co) can be separated from the precipitate through the ammonia permeation step, and the recovery rate of the valuable metals can be improved.

[0061] (8) Solvent extraction step S80

[0062] In the solvent extraction step S80, each metal component (Ni and / or Co) is extracted from the metal solution by solvent extraction. In addition, in the solvent extraction step S80, other metal components (such as Al) remaining in the metal solution can also be separated. Specifically, Figure 4 As shown, the solvent extraction step S80 in this embodiment includes a Co extraction step S81 and a Ni extraction step S82. Thus, a Co solution and a Ni solution can be prepared respectively. However, the solvent extraction step S80 can be appropriately added, changed, or deleted according to the metal components contained in the metal solution. The following is a specific description.

[0063] (8-1) Co extraction step S81

[0064] In the Co extraction step S81, an organic solvent (first extract) having high extractability for Co and low extractability for Li, Al, Cu, and Ni is added to the metal solution. In this way, Co can be separated from the metal solution, and a Co solution in which Co is dissolved in the first extract can be obtained. It should be noted that specific examples of the first extract include phosphonates such as 2-ethylhexylphosphonate (PC-88A) and the like. In addition, the first extract can also use an extract obtained by mixing and diluting these extractants. Then, in the Co extraction step S81, the metal solution and the first extract are stirred and suspended. As a result, the Co in the metal solution is dissolved in the first extract. Then, by standing until the two liquids are separated, a Co solution in which Co is dissolved in the first extract and a metal solution from which Co has been removed can be obtained.

[0065] In the Co extraction step S81, the extracted Co solution (the first extract containing Co) may be subjected to a stripping treatment. In the stripping treatment, first, the Co solution (organic phase) and the acidic aqueous solution are stirred and mixed using a mixer or the like. Then, the mixture is allowed to stand until the two liquids are separated. Thus, an aqueous Co solution may be obtained. It should be noted that as the acidic aqueous solution used in the stripping treatment, sulfuric acid, hydrochloric acid, etc. (particularly sulfuric acid) may be cited.

[0066] (8-2) Ni extraction step S82

[0067] In the Ni extraction step S82, an organic solvent (second extract) having high Ni extractability and low Li, Al, and Cu extractability is added to the metal solution. Thus, Ni can be separated from the metal solution, and a Ni solution in which Ni is dissolved in the second extract can be obtained. It should be noted that as a specific example of the second extract, carboxylic acid extractants such as neodecanoic acid and cyclohexane acid can be cited. In addition, the extracted Ni solution (the second extract containing Ni) can also be subjected to a back extraction treatment. Thus, an aqueous Ni solution can be obtained. It should be noted that since the steps of the back extraction treatment have been described, repeated records are omitted.

[0068] (9) Li crystallization step S90

[0069] In the Li crystallization step S90, crystals of Li compounds are precipitated from the metal solution after the solvent extraction step S80. In the Li crystallization step S90, a previously known crystallization treatment can be used without particular restrictions. For example, in the Li crystallization step S90, sodium carbonate can be added to the metal solution. Thus, crystals of lithium carbonate (Li2CO3) can be precipitated. It should be noted that the Li compound generated in the Li crystallization step S90 is not limited to lithium carbonate. For example, lithium hydroxide (LiOH) can be generated as a Li compound as needed. In the generation of the lithium hydroxide, first, the lithium carbonate precipitated from the metal solution is dissolved (or suspended) in a prescribed solvent. Then, calcium hydroxide is added to the solution. Then, the solvent is evaporated and removed as needed. Thus, crystals of lithium hydroxide can be precipitated. However, in the manufacturing method disclosed herein, the Li crystallization step S90 is not necessary. For example, when the metal solution does not contain Li (in other words, when the recovery object does not contain Li), the Li crystallization step S90 can also be omitted.

[0070] (10) Precursor production step S100

[0071] In the precursor preparation step S100, a positive electrode active material precursor (metal composite hydroxide) is prepared. In the precursor preparation step S100, a previously known method (such as a crystallization method, etc.) can be used without particular restrictions. For example, an aqueous solution containing a metal element source (typically a water-soluble ionic compound) is prepared. Next, the prepared aqueous solution containing the metal element source and an alkaline solution (such as an ammonia solution, etc.) are mixed in a reaction tank, and the pH of the mixed solution is controlled while stirring, thereby coprecipitating and crystallizing the particles of the metal composite hydroxide in the reaction tank, thereby implementing. Here, in this embodiment, the ammonia seepage solution obtained in the ammonia seepage step S70 can be appropriately used as the above-mentioned alkaline solution. The ammonia seepage solution contains Ni and / or Co in the ammonia solution. Therefore, the above-mentioned ammonia seepage solution can be directly used as the alkaline solution of the precursor preparation step S100 without the need for treatment such as cleaning. Therefore, Co and Ni in the ammonia solution can also be crystallized as positive electrode active material precursors. That is, the valuable metals (Ni and / or Co) recovered from the precipitate in the ammonia seepage step S70 can be effectively used.

[0072] It should be noted that, as described above, crystallization is performed while controlling the pH of the mixed solution in the precursor preparation step S100. At this time, an alkaline solution (NH3 aqueous solution, NaOH aqueous solution, etc.) for preparing the pH can be added dropwise to the reaction tank. It should be noted that the amount of Ni and Co in the metal solution obtained in the ammonia seepage step S70 can be obtained by ICP analysis. Therefore, depending on the composition of the target positive electrode active material, metal components such as Ni, Co or other Mn can be added. The metal component can be added in the form of a metal sulfate, a hydrate, etc. In addition, in this case, various metal components obtained in the solvent extraction step S80 can be used as metal components.

[0073] (11) Active Material Generation Step S110

[0074] In the active material generation step S110, the metal compound and Li compound (such as Li2CO3, etc.) obtained in the precursor preparation step S100 are used to generate a battery material (positive electrode active material). For example, the positive electrode active material precursor (metal composite hydroxide) obtained in the above-mentioned precursor preparation step S100 and the Li compound are mixed, and the mixture is calcined. In this way, the positive electrode active material (lithium transition metal composite oxide) of the lithium ion secondary battery can be manufactured. It should be noted that the Li compound obtained in the Li crystallization step S90 can be used as the Li compound.

[0075] The above is a description of the manufacturing method of the battery material of the present embodiment. As described above, in the manufacturing method of the present embodiment, an ammonia seepage process is performed in which the precipitate obtained by the neutralization precipitation process is immersed in an ammonia solution. Thus, Ni and / or Co contained in the precipitate can be dissolved in the ammonia solution to obtain an ammonia seepage solution containing Ni and / or Co. Therefore, the valuable metals (Ni and / or Co) precipitated as part of the precipitate during the neutralization precipitation process can be appropriately recovered (manufactured). In other words, the recovery rate of the valuable metals can be improved. In addition, the ammonia seepage solution obtained by the manufacturing method disclosed herein can be directly used in the precursor preparation step S100, for example, without performing steps such as washing. Thus, the valuable metals (Ni and / or Co) contained in the ammonia seepage solution can be used as a positive electrode active material precursor. Therefore, the valuable metals (Ni and / or Co) can be efficiently recovered, and the recovery rate of the valuable metals can be greatly improved.

[0076] 3. Other Implementation Methods

[0077] An embodiment of the technology disclosed herein has been described above. It should be noted that the technology disclosed herein is not limited to the above embodiment, and includes other embodiments in which various configurations are changed. Other examples of the embodiments of the technology disclosed herein will be described below.

[0078] (a) Changes in the solvent extraction process

[0079] The specific processing steps in the solvent extraction step S80 can be appropriately changed. For example, the solvent extraction step S80 in the above embodiment includes a Co extraction step and a Ni extraction step. Thus, the Co solution and the Ni solution can be extracted separately. However, in the solvent extraction step S80, Ni and Co can also be extracted at the same time. Thus, it is possible to improve the manufacturing efficiency by shortening the process.

[0080] In addition, the steps that can be included in the solvent extraction step S80 are not limited to the above-mentioned Co extraction step and Ni extraction step. For example, in the case where manganese (Mn) is further included in the metal solution as a metal component, a Mn extraction step of extracting Mn from the metal solution can be further included in the solvent extraction step S80. The method of the Mn extraction step is not particularly limited, and can be performed by adding an organic solvent (third extracting liquid) having high extractability for Mn and low extractability for Li, Al, Cu, Co, and Ni to the metal solution. As the third extracting liquid, a phosphate ester extractant, an oxime extractant, etc. can be used. As a specific example of a phosphate ester extractant, di-2-ethylhexyl phosphate (D2EHPA) and the like are included. In addition, as a specific example of an oxime extractant, 2-hydroxy-5-nonyl acetophenone oxime (LIX84), 5-dodecyl salicylaldehyde oxime (LIX860), 5-nonyl salicylaldehyde oxime (ACORGA M5640), etc. can be cited. In addition, the third extract may be a mixture of these extractants and diluted extracts. In addition, the Mn solution (third extract containing Mn) after extraction may be subjected to a stripping treatment. It should be noted that the specific extraction method and stripping treatment method may be the same as those in the above-mentioned Co extraction step S81 and Ni extraction step S82, and therefore are omitted here.

[0081] (b) Omission of solvent extraction step

[0082] In addition, according to the manufacturing method disclosed herein, the solvent extraction step S80 can also be omitted. Specifically, as described above, in the technology disclosed herein, Al can be separated from the metal solution by the neutralization precipitation step S50. Therefore, a solution containing high-purity valuable metals (Ni and / or Co) can be formed. Therefore, in the case of using a recycling object that does not contain Cu, such as an engineering end material of the positive electrode plate 30, the mixed solution of valuable metals used in the precursor production step S100 (an aqueous solution containing a metal element source) can be obtained without performing the solvent extraction step S80.

[0083] On the other hand, in the case where Li is contained in the metal solution, the following method can be cited as an example of a method for recovering Li. First, when performing the roasting step S20, a non-metallic chlorine compound (HCl, etc.) is added to the recovery object for roasting. As a result, the Li in the recovery object reacts with the non-metallic chlorine compound to generate LiCl. Next, a water permeation step of immersing the roasted recovery object in water is performed. Since the above-mentioned LiCl is a water-soluble compound, Li can be recovered only by contacting the recovery object with water. In this way, Li in the metal solution can be recovered (manufactured), and a mixed solution of valuable metals (an aqueous solution containing a metal element source) used in the precursor preparation step S100 can be obtained without performing the solvent extraction step S80. That is, the description involved in the above-mentioned embodiment is not intended to limit each process. In the manufacturing method disclosed herein, each process can be appropriately added, deleted, or changed as needed.

[0084] (c) Addition of Li separation step

[0085] In addition, in some embodiments, the Li separation process can also be performed on the metal solution after the solvent extraction process S80. The Li separation process is a process for further removing Cu and Al from the metal solution to prepare a high-concentration Li solution. Thus, a high-purity Li compound can be obtained in the Li crystallization process S90. It should be noted that the method for preparing the Li solution is not particularly limited, and it is preferred to appropriately adopt a previously known method such as a solvent extraction method and an ion exchange method. It should be noted that only the evaporation of the solvent can be performed instead of the Li concentration process. In this case, a high-concentration Li solution can also be obtained.

[0086] (d) Addition of Li Concentration Step

[0087] In addition, the Li concentration process may be performed on the metal solution after the above-mentioned Li separation process. In the Li concentration process, the Li solution is heated to evaporate the solvent. Thus, a high-concentration Li solution can be obtained, so the crystallization efficiency in the Li crystallization process S90 can be improved. It should be noted that the Li concentration process may also be performed on the metal solution that has not undergone the Li separation process. In this case, a high-concentration Li solution can also be obtained.

[0088] [Test example]

[0089] Hereinafter, test examples related to the technology disclosed herein will be described. It should be noted that the contents of the test examples described below are not intended to limit the technology disclosed herein.

[0090] <Test Example 1: Study on pH during the neutralization precipitation step>

[0091] (Example 1)

[0092] [Sample preparation]

[0093] In this experiment, the positive electrode plate was used as the recycling object, and the following process was performed on the recycling object. Specifically, as the positive electrode plate, a positive electrode plate with a positive electrode active material layer coated on the surface of the positive electrode core (Al foil) was used. It should be noted that the positive electrode active material in this experiment was lithium nickel cobalt manganese composite oxide (LiNi 1 / 3 Co 1 / 3 Mn 1 / 3 O2). Then, the positive electrode plate was crushed and passed through a sieve with a mesh size of 500 μm, and the obtained powder was used as a test sample. It should be noted that the powder of the test sample was analyzed by ICP, and the mass ratio of Al in the sample to the total amount of Ni and Co was 4 wt%.

[0094] [Acid seepage process]

[0095] Next, the test sample and a mixture (pH 0.01) of sulfuric acid (H2SO4) (concentration 2 mol / L) as an acid solution and hydrogen peroxide (H2O2) (concentration 0.6 mol / L) as a reducing agent were mixed. Then, the acid solution was maintained at 80°C and stirred at a stirring speed of 600 rpm for 6 hours. After stirring, the acid exudate was filtered, and the obtained acid exudate was analyzed by ICP to determine the amount of each of Al, Ni, and Co. It should be noted that the result of the above ICP measurement was that the concentration of Ni and Co in the acid exudate (the sum of Ni and Co) was 1.0 mol / L.

[0096] [Neutralization precipitation process]

[0097] The acid exudate obtained above was maintained at 25° C. and stirred at a stirring speed of 600 rpm, while 10 wt % sodium hydroxide solution was added dropwise to the acid exudate. When the pH of the acid exudate reached 5.1, the addition of sodium hydroxide was stopped. After the addition was stopped, stirring was continued for 10 minutes at a stirring speed of 600 rpm to confirm that the pH did not change. Then, the metal solution and the precipitate were separated into solid and liquid by filtration.

[0098] (Example 2)

[0099] In the neutralization precipitation step, the addition of sodium hydroxide was stopped when the pH of the acid permeate reached 5.6. Other than that, the same procedures were followed as in Example 1.

[0100] (Example 3)

[0101] In the neutralization precipitation step, the addition of sodium hydroxide was stopped when the pH of the acid permeate reached 6.2. Other than that, the same procedures were followed as in Example 1.

[0102] [Residual rate of metal solution in the neutralization precipitation process]

[0103] The residual rates of valuable metals (Ni, Co) and Al in the metal solution of each example after the neutralization precipitation step were calculated. Specifically, first, the amounts of Ni, Co and Al in the metal solution were measured by subjecting the metal solution to ICP. Then, the residual rates of Ni and Co in the metal solution and the residual rate of Al in the metal solution compared with the acid leaching solution of each example (i.e., before the neutralization precipitation step) were calculated based on the following formulas (1) and (2). The results are shown in Table 1.

[0104] Residual rate of Ni and Co in the metal solution (%) = {(Ni mass in the metal solution + Co mass in the metal solution) / (Ni mass in the acid leaching solution + Co mass in the acid leaching solution)} × 100…(1)

[0105] Residual Al rate in metal solution (%) = (amount of Al in metal solution / amount of Al in acid leaching solution) × 100 (2)

[0106] [Ni / Co Ratio in the Precipitate in the Neutralization Precipitation Step]

[0107] In addition, the ratio of the amount of valuable metals (Ni, Co) to the amount of Al in the precipitate of each example after the neutralization precipitation step was calculated. Specifically, first, the amount of Ni, Co and Al in the precipitate was measured by performing ICP on the precipitate after the neutralization precipitation step. Then, the ratio of the amount of valuable metals (Ni, Co) in the precipitate of each example was calculated based on the following formula (3). The results are shown in Table 1.

[0108] Ni / Co ratio in precipitate (%) = {(Ni mass in precipitate + Co mass in precipitate) / Al mass in precipitate} × 100 (3)

[0109] [Table 1]

[0110]

[0111] As shown in the results of Table 1, in the neutralization precipitation process, in Example 1 where the pH during precipitation was 5.1, the Al residual rate in the metal solution was 1.5%. It can be seen that when the pH of the acid effluent is neutralized to 5.1, the Al contained in the acid effluent can be substantially neutralized and precipitated. Comparing Examples 1 to 3, the higher the pH during precipitation, the lower the Al residual rate in the metal solution, and in Example 3 where the pH during precipitation was 6.2, the Al residual rate in the metal solution was the lowest. On the other hand, in Example 3, the Ni and Co residual rates in the metal solution were the lowest, and the Ni and Co ratios in the precipitate were also the highest.

[0112] <Test Example 2: Study of Ammonia Leakage Process>

[0113] (Example 4)

[0114] [Ammonia seepage process]

[0115] The precipitate obtained by the above-mentioned neutralization precipitation step is subjected to ammonia seepage. Specifically, first, an ammonia solution with a pH of 11.2 (ammonia concentration in the solution is 1.5 wt%) is prepared. Then, the precipitate of Example 1 obtained by the above-mentioned neutralization precipitation step is placed in the ammonia solution. Then, the ammonia solution is maintained at 80°C and stirred at a stirring speed of 600 rpm for 2 hours. It should be noted that when a decrease in the pH in the solution is observed during stirring, the pH is adjusted to 11.2 by adding an additional ammonia solution with an ammonia concentration of 28 wt%. After stirring, the ammonia seepage solution and the residue are separated into solid and liquid by filtration.

[0116] (Example 5)

[0117] In Example 5, the ammonia seepage step was performed with the pH of the ammonia solution being 12.1 (ammonia concentration in the solution: 10.0 wt %). Other than that, the same procedures were followed as in Example 4.

[0118] (Example 6)

[0119] In Example 6, 2 mol / L of ammonium sulfate ((NH4)2SO4) as a pH buffer material was added to ammonia water with a pH of 12.1 (ammonia concentration in the solution 10.0 wt%) as an ammonia solution. Thus, the pH of the ammonia solution was set to 9.6 for the ammonia seepage step. Other than that, the same procedures were followed as in Example 4.

[0120] (Example 7~Example 9)

[0121] In Example 7, the ammonia seepage step was performed using the precipitate of Example 2. Other than that, the same procedures were followed as in Example 4.

[0122] In Example 8, the ammonia seepage step was performed using the precipitate of Example 2. Other than that, the same procedures were followed as in Example 5.

[0123] In Example 9, the ammonia seepage step was performed using the precipitate of Example 2. Other than that, the same procedures were followed as in Example 6.

[0124] (Example 10~Example 12)

[0125] In Example 10, the ammonia seepage step was carried out using the precipitate of Example 3. Other than that, the same procedures were followed as in Example 4.

[0126] In Example 11, the ammonia seepage step was carried out using the precipitate of Example 3. Other than that, the same procedures were followed as in Example 5.

[0127] In Example 12, the ammonia seepage step was carried out using the precipitate of Example 3. Other than that, the same procedures were followed as in Example 6.

[0128] (Example 13)

[0129] In Example 13, the ammonia seepage step was performed while the temperature of the ammonia solution was maintained at 25° C. Other than this, the same procedures were followed as in Example 12.

[0130] [Ni and Co residual ratio in the residue]

[0131] The residual rate of the valuable metals (Ni, Co) in the residue of each example after the ammonia seepage process was calculated. Specifically, first, the amount of Ni, Co and Al in the residue was measured by performing ICP on the residue. Then, the ratio of the amount of the valuable metals (Ni, Co) in the residue of each example to the amount of Al in the residue was calculated based on the following formula (4). The results are shown in Table 2.

[0132] Ni / Co ratio in the residue (%) = {(Ni mass in the residue + Co mass in the residue) / Al mass in the residue} × 100 (4)

[0133] [Al seepage rate in ammonia seepage solution]

[0134] The Al seepage rate in the ammonia seepage solution of each example after the ammonia seepage process was calculated. Specifically, first, the amount of Al in the ammonia seepage solution was measured by performing ICP on the ammonia seepage solution. Then, the ratio of the amount of Al in the ammonia seepage solution of each example to the amount of Al in the residue was calculated based on the following formula (5). The results are shown in Table 2.

[0135] Al seepage rate in ammonia seepage solution (%) = (amount of Al in ammonia seepage solution / amount of Al in residue) × 100…(5)

[0136] [Table 2]

[0137]

[0138] As shown in the results of Table 2, in Example 4 in which the pH of the ammonia solution was set to 11.2, the ratio of Ni to Co in the residue was significantly reduced compared to the ratio of Ni to Co in the precipitate (i.e., before the ammonia seepage process). In addition, the Al seepage rate in the ammonia seepage solution of Example 4 was 0.2%. It can be seen from this that in Example 4, Ni and Co in the precipitate were appropriately and selectively recovered by ammonia seepage. On the other hand, as shown in Example 5, when the pH of the ammonia solution was set to 12.1, the recovery effect of Ni and Co in the precipitate caused by ammonia seepage was observed, and the Al seepage rate in the ammonia seepage solution was higher than that in Example 4. In addition, comparing Examples 4 to 6, in Example 6 in which ammonium sulfate was contained in the ammonia solution, the Al seepage rate in the ammonia seepage solution was the lowest, and the ratio of Ni to Co in the residue was the lowest.

[0139] As shown in the results of Examples 7 to 9 and Examples 10 to 12, it can be seen that even when the precipitates of Examples 2 and 3, which have different pH values ​​during neutralization and precipitation, are used, the same results as those of Examples 4 to 6 can be obtained. From the results of Example 13, it can be seen that even when the temperature of the ammonia solution is 25°C, Ni and Co can be selectively recovered from the precipitate, and the seepage of Al into the ammonia seepage solution can be suppressed. Comparing Examples 12 and 13, the ratio of Ni to Co in the residue of Example 12, in which the temperature of the ammonia solution is 80°C, is lower.

[0140] The above detailed description of the technology disclosed herein is for illustration only and does not limit the scope of the patent claims. The technology described in the scope of the patent claims includes various deformations and changes to the specific examples illustrated above. That is, the technology disclosed herein includes the forms described in the following items 1 to 7.

[0141] <Project 1>

[0142] A method for manufacturing a battery material, comprising:

[0143] A preparation step of preparing a recycling object including at least one of Ni and Co;

[0144] an acid seepage step, wherein the object to be recovered is immersed in an acid solution to obtain an acid seepage solution;

[0145] A neutralization precipitation step, mixing the acid exudate with a neutralizer to obtain a precipitate;

[0146] a solid-liquid separation step, separating the precipitate into solid and liquid; and

[0147] The ammonia seepage step is to immerse the separated precipitate in an ammonia solution containing ammonium ions to obtain an ammonia seepage solution containing at least one of the Ni and the Co.

[0148] <Project 2>

[0149] The method for producing a battery material according to item 1, wherein the pH of the ammonia solution is adjusted to 9.0 to 11.5 before the ammonia seepage step is performed.

[0150] <Project 3>

[0151] The method for producing a battery material according to item 1 or 2, wherein the ammonia solution contains at least one selected from ammonium sulfate, ammonium chloride, and ammonium acetate.

[0152] <Item 4>

[0153] The method for producing a battery material according to any one of items 1 to 3, further comprising a precursor preparation step of preparing a positive electrode active material precursor using the ammonia permeate obtained in the ammonia permeation step.

[0154] <Item 5>

[0155] The method for producing a battery material according to any one of items 1 to 4, wherein the ammonia seeping step is performed at a temperature of the ammonia solution of 25 to 100°C.

[0156] <Item 6>

[0157] The method for producing a battery material according to any one of items 1 to 5, wherein in the neutralization precipitation step, the pH of the acid effluent is neutralized to 5.0 to 6.5.

[0158] <Item 7>

[0159] A method for manufacturing a battery material according to any one of items 1 to 6, wherein the recycling object includes at least one selected from lithium nickel composite oxide, lithium cobalt composite oxide, lithium nickel manganese composite oxide, lithium manganese cobalt composite oxide, lithium nickel cobalt composite oxide, and lithium nickel manganese cobalt composite oxide.

Claims

1. A method for manufacturing a battery material, comprising: A preparation step of preparing a recycling object including at least one of Ni and Co; an acid seepage step, immersing the recovery object in an acid solution to obtain an acid seepage solution; a neutralization precipitation step, mixing the acid exudate with a neutralizer to obtain a precipitate; A solid-liquid separation step, separating the precipitate into solid and liquid; as well as The ammonia seepage step includes immersing the separated precipitate in an ammonia solution containing ammonium ions to obtain an ammonia seepage solution containing at least one of the Ni and the Co.

2. The method for producing a battery material according to claim 1, wherein: The pH of the ammonia solution is adjusted to 9.0 to 11.5, and the ammonia seepage step is performed.

3. The method for producing a battery material according to claim 1 or 2, wherein: The ammonia solution contains at least one selected from ammonium sulfate, ammonium chloride and ammonium acetate.

4. The method for producing a battery material according to claim 1 or 2, wherein: Further including: The precursor preparation step is to prepare a positive electrode active material precursor using the ammonia permeate obtained in the ammonia permeation step.

5. The method for producing a battery material according to claim 1 or 2, wherein: The ammonia seeping step is performed by setting the temperature of the ammonia solution to 25 to 100°C.

6. The method for producing a battery material according to claim 1 or 2, wherein: In the neutralization precipitation step, the pH of the acid exudate is neutralized to 5.0 to 6.

5.

7. The method for producing a battery material according to claim 1 or 2, wherein: The recycling object includes at least one selected from lithium nickel composite oxide, lithium cobalt composite oxide, lithium nickel manganese composite oxide, lithium manganese cobalt composite oxide, lithium nickel cobalt composite oxide, and lithium nickel manganese cobalt composite oxide.

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