Method for leaching valuable metals from waste lithium ion battery

Abstract

The present invention relates to a method for leaching valuable metals from spent lithium-ion batteries. A method for leaching valuable metals from a lithium-ion battery according to one embodiment comprises: a spent lithium-ion battery black mass preparation step (S10) in which a spent lithium-ion battery black mass in powder form is prepared by undergoing a pretreatment process of crushing the spent lithium-ion battery; a copper leaching step (S20) in which copper contained in the spent lithium-ion battery black mass is selectively leached out and recovered in its entirety using ammonia water having a set concentration and temperature; and a valuable metal leaching step (S30) using ammonium persulfate / distilled water in which ammonium persulfate ((NH4)2S2O8) is added to the residue after the copper has been completely leached out in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached out and recovered using distilled water as a leaching agent.

Description

Technology Field

[0001] The embodiments of the present invention relate to a method for leaching valuable metals from spent lithium-ion batteries, and more specifically, to an economical and environmentally friendly method for leaching valuable metals from spent lithium-ion batteries that can selectively leach copper and valuable metals such as Ni, Co, Mn, and Li from spent lithium-ion batteries using an ammonia, H2O-(NH4)2S2O8 leaching process. Background Technology

[0002] As is well known, lithium-ion batteries are widely used as power sources in various product and technology fields due to their high energy density and lightweight characteristics.

[0003] A lithium-ion battery can be composed of a cathode material, a negative electrode material, an electrolyte, and a separator. Lithium-ion batteries are classified as high-performance secondary batteries that can be reused after charging, and they can be charged and discharged and have a relatively long lifespan.

[0004] However, since lithium-ion batteries are consumables that are discarded after their lifespan ends, the amount of waste is increasing along with the recent rise in their usage.

[0005] However, spent lithium-ion batteries are recognized as economically valuable waste resources because they have simple properties and contain large amounts of valuable metals such as lithium and cobalt, which are relatively expensive.

[0006] Therefore, recently, active technological development is underway for the recycling of spent lithium-ion batteries, which enables the efficient use of resources by recovering and recycling high-value precious metals from batteries that have reached the end of their lifespan and are being discarded.

[0007] The previously introduced method for recovering lithium and valuable metals from spent lithium-ion batteries utilized a method of recovering lithium after recovering the valuable metals.

[0008] However, when lithium is recovered after the valuable metal recovery process, the concentration of recoverable lithium is significantly reduced. In addition, when lithium is recovered after the valuable metal recovery process, the sodium concentration in the mixture after the process increases due to the sodium added during the intermediate process, so there is a problem in that the recovered lithium cannot meet the quality standards for use as a battery raw material.

[0009] Meanwhile, recently, a method utilizing a sulfuric acid and hydrogen peroxide reduction leaching process has been introduced as one of the methods for recovering valuable metals from spent lithium-ion batteries. However, this method has disadvantages in terms of energy consumption due to the excessive use of sulfuric acid and the fact that it is an atmospheric pressure heating leaching process, as well as the problem of solution ejection caused by the addition of hydrogen peroxide. Furthermore, since impurities (Fe, Al, etc.) remain in the leaching solution after leaching, a precipitation process is required to remove them, and in some cases, copper (Cu) is also considered an impurity rather than a recoverable material and must be removed.

[0010] Therefore, there is a need to develop a technology that can resolve various problems arising from conventional methods and selectively leach valuable metals from impurities (Fe, Al, etc.) in spent lithium-ion batteries using an eco-friendly, low-energy process.

[0011] As related prior art, there is Korean Patent Publication No. 10-2007-0046990 (hereinafter referred to as the prior art), and the said prior art discloses a technology regarding a method for recovering valuable metals from spent lithium-ion batteries. Prior art literature

[0012] Republic of Korea Published Patent Application No. 10-2007-0046990 The problem to be solved

[0013] To solve the above problems, the present invention aims to provide a method for leaching valuable metals from spent lithium-ion batteries, which can selectively leach copper and valuable metals such as Ni, Co, Mn, and Li from spent lithium-ion batteries using an ammonia, H2O-(NH4)2S2O8 leaching process.

[0014] In addition, the present invention aims to provide a method for leaching valuable metals from spent lithium-ion batteries, which can recover copper from spent lithium-ion batteries using ammonia water and leach valuable metals such as Ni, Co, Mn, and Li from the residue generated after copper recovery.

[0015] In addition, the present invention aims to provide a method for leaching valuable metals from spent lithium-ion batteries, which has the advantages of being very economical and environmentally friendly, as the leaching process can be carried out using both distilled water and room temperature leaching.

[0016] The objects of the present invention are not limited to those mentioned above, and other unmentioned objects and advantages of the present invention may be understood from the following description and will be more clearly understood by the embodiments of the present invention. Furthermore, it will be readily apparent that the objects and advantages of the present invention can be realized by the means and combinations thereof set forth in the claims. means of solving the problem

[0017] To achieve the above objective, the present invention can provide a method for leaching copper and valuable metals from spent lithium-ion batteries according to various embodiments. In particular, the present invention can provide a method for leaching valuable metals from spent lithium-ion batteries, which can selectively leach copper and valuable metals such as Ni, Co, Mn, and Li from spent lithium-ion batteries using an ammonia, H2O-(NH4)2S2O8 leaching process.

[0018] A method for leaching valuable metals from a spent lithium-ion battery according to an embodiment of the present invention comprises: a spent lithium-ion battery black mass preparation step (S10) in which a spent lithium-ion battery black mass in powder form is prepared by undergoing a pretreatment process of crushing the spent lithium-ion battery; a copper leaching step (S20) in which copper contained in the spent lithium-ion battery black mass is selectively leached out and recovered in its entirety using ammonia water having a set concentration and temperature; and a valuable metal leaching step (S30) using ammonium persulfate / distilled water in which ammonium persulfate ((NH4)2S2O8) is added to the residue after the copper has been completely leached out in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached out and recovered using distilled water as a leaching agent.

[0019] In the method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention, in the waste lithium-ion battery black mass preparation step (S10), at least two types of waste lithium-ion batteries may be mixed among those in which the ratio of nickel (Ni):cobalt (Co):manganese (Mn), which is the composition of the positive electrode active material content of the battery, is 1:1:1, 5:3:2, 6:2:2, or 8:1:1.

[0020] The method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention can leach out all of the copper contained in the black mass of the waste lithium-ion battery by using an ammonia water solution of 100 vol.% and 45°C at a stirring speed of 150 rpm in the copper leaching step (S20).

[0021] A method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention further includes, after the copper leaching step (S20), a step (S21) of recovering a copper solution by separating the leaching solution from solid to liquid in which the copper has been completely leached out.

[0022] In the method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention, when ammonium persulfate ((NH4)2S2O8) is added to the residue after the copper has been completely leached in the valuable metal leaching step (S30) using ammonium persulfate / distilled water, the amount of ammonium persulfate ((NH4)2S2O8) added can be at least twice the amount of the sample.

[0023] A method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention, by undergoing the valuable metal leaching step (S30) using ammonium persulfate / distilled water, may have a leaching rate of at least 90% for nickel (Ni) and a leaching rate of less than 60% for cobalt (Co), manganese (Mn), and lithium (Li).

[0024] In a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention, the valuable metal leaching step (S30) using ammonium persulfate / distilled water may include: a first valuable metal leaching step (S31) in which ammonium persulfate ((NH4)2S2O8) is first introduced in a set weight ratio to the residue after the copper has been completely leached, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are first leached; and a second valuable metal leaching step (S32) in which, after the first valuable metal leaching step (S31), ammonium persulfate ((NH4)2S2O8) is secondarily introduced in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are secondarily leached.

[0025] In a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention, the valuable metal leaching step (S30) using ammonium persulfate / distilled water may further include a third valuable metal leaching step (S33) in which ammonium persulfate ((NH4)2S2O8) is added in a set weight ratio after the second valuable metal leaching step (S32) and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached for the third time. Effects of the invention

[0026] According to the method for leaching valuable metals from spent lithium-ion batteries of the present invention, copper can be recovered using ammonia water, and there is an advantage in that valuable metals such as Ni, Co, Mn, and Li can be selectively leached from the residue generated after copper recovery.

[0027] Furthermore, according to the method for leaching valuable metals from spent lithium-ion batteries of the present invention, all processes can be carried out under distilled water and room temperature leaching. Accordingly, it has the advantages of being economical and environmentally friendly.

[0028] In addition to the effects described above, the specific effects of the present invention are described together with the specific details for implementing the invention below. Brief explanation of the drawing

[0029] FIG. 1 is a flowchart briefly illustrating a method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention. FIG. 2 is a flowchart briefly illustrating the detailed steps of the valuable metal leaching step (S30) using ammonium persulfate / distilled water in the method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention. FIG. 3 is a simplified process diagram illustrating a method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention. Figure 4 is a table showing the content of valuable metals in the black mass of a waste lithium-ion battery in a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention. FIG. 5 is a table showing the leaching rate of valuable metals, % (solid-liquid ratio: 0.5 / 10, 45℃, 150rpm) according to the ammonia water concentration in a method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention. FIG. 6 is a table showing the leaching rate of valuable metals using ammonia according to temperature, % (solid-liquid ratio: 0.5 / 10, 100 vol.% 150 rpm) in a method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention. FIG. 7 is a table showing the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system in the method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 1:1). FIG. 8 is a table showing the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system in the method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 2:1). FIG. 9 is a table showing the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system in the method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 4:1). Specific details for implementing the invention

[0030] Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings so that those skilled in the art can easily implement the invention. The present invention may be embodied in various different forms and is not limited to the embodiments described herein.

[0031] To clearly explain the present invention, parts unrelated to the description have been omitted, and the same reference numerals are assigned to identical or similar components throughout the specification. Furthermore, some embodiments of the present invention are described in detail with reference to the exemplary drawings. In assigning reference numerals to the components of each drawing, identical components may have the same reference numeral whenever possible, even if they are shown in different drawings. Additionally, in describing the present invention, if it is determined that a detailed description of related known components or functions could obscure the essence of the present invention, such detailed description may be omitted.

[0032] In describing the components of the present invention, terms such as first, second, A, B, (a), (b), etc., may be used. These terms are intended merely to distinguish the components from other components, and the nature, order, sequence, or number of the components are not limited by these terms. Where it is stated that a component is "connected," "combined," or "joined" to another component, it should be understood that the component may be directly connected or joined to the other component, but that other components may be "interposed" between each component, or that each component may be "connected," "combined," or "joined" through other components.

[0033] In addition, for convenience of explanation in implementing the present invention, the components may be described in detail; however, these components may be implemented within a single device or module, or a single component may be divided and implemented across multiple devices or modules.

[0034] Hereinafter, a method for leaching valuable metals from waste lithium-ion batteries according to an embodiment of the present invention will be described in detail with reference to the attached drawings.

[0035] FIG. 1 is a flowchart briefly illustrating a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention, FIG. 2 is a flowchart briefly illustrating detailed steps of a step (S30) for leaching valuable metals using ammonium persulfate / distilled water, and FIG. 3 is a process diagram briefly illustrating a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention.

[0036] The present invention provides a method for leaching valuable metals from spent lithium-ion batteries, which can selectively leach copper and valuable metals such as Ni, Co, Mn, and Li using an ammonia, H2O-(NH4)2S2O8 leaching process. Copper can be fully leached and recovered from spent lithium-ion batteries using ammonia water, and valuable metals such as Ni, Co, Mn, and Li can be leached from the residue remaining after copper recovery. As such, the present invention is highly economical and environmentally friendly, as the valuable metal leaching process can be carried out using distilled water or under room temperature leaching conditions.

[0037] Referring to FIGS. 1 to 3, a method for leaching valuable metals from a waste lithium-ion battery according to an embodiment of the present invention includes a waste lithium-ion battery black mass preparation step (S10), a copper leaching step (S20), and a valuable metal leaching step using ammonium persulfate / distilled water (S30).

[0038] In the waste lithium-ion battery black mass preparation step (S10), waste lithium-ion battery black mass in powder form can be prepared by undergoing a pretreatment process of crushing, grinding, and classifying residual materials from waste lithium-ion batteries.

[0039] In the copper leaching step (S20), the copper contained in the spent lithium-ion battery black mass can be selectively leached out and recovered in its entirety using ammonia water having a set concentration and temperature.

[0040] In the valuable metal leaching step (S30) using ammonium persulfate / distilled water, ammonium persulfate ((NH4)2S2O8) is added to the residue (or sample) after the copper has been completely leached in the previous step in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) can be leached and recovered using distilled water as a leaching agent.

[0041] A method for leaching valuable metals from a spent lithium-ion battery according to a preferred embodiment may, in the spent lithium-ion battery black mass preparation step (S10), at least two types of spent lithium-ion batteries may be mixed among those in which the ratio of nickel (Ni):cobalt (Co):manganese (Mn), which is the composition of the positive electrode active material content of the battery, is 1:1:1, 5:3:2, 6:2:2, or 8:1:1.

[0042] According to a preferred embodiment, the method for leaching valuable metals from a spent lithium-ion battery can, in the copper leaching step (S20), use an ammonia solution of 100 vol.% and 45°C at 150 rpm to leach out all the copper contained in the spent lithium-ion battery black mass.

[0043] A method for leaching valuable metals from a waste lithium-ion battery according to a preferred embodiment may further include, after the copper leaching step (S20), a step (S21) of recovering a copper solution by separating the leaching solution from solid to liquid in which the copper has been completely leached out (see FIG. 3).

[0044] In a method for leaching valuable metals from a waste lithium-ion battery according to a preferred embodiment, when ammonium persulfate ((NH4)2S2O8) is added to the residue after the copper has been completely leached in the valuable metal leaching step (S30) using ammonium persulfate / distilled water, the amount of ammonium persulfate ((NH4)2S2O8) added can be at least twice the amount of the sample.

[0045] A method for leaching valuable metals from a spent lithium-ion battery according to a preferred embodiment can have a leaching step (S30) using ammonium persulfate / distilled water, wherein nickel (Ni) has a leaching rate of at least 90%, and cobalt (Co), manganese (Mn), and lithium (Li) have a leaching rate of 60% to less than 90%.

[0046] In a method for leaching valuable metals from a spent lithium-ion battery according to a preferred embodiment, the valuable metal leaching step (S30) using ammonium persulfate / distilled water may include first to third valuable metal leaching steps (S31, S32, S33).

[0047] In the first valuable metal leaching step (S31), ammonium persulfate ((NH4)2S2O8) is first added to the residue after the copper has been completely leached out in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) can be first leached out.

[0048] In the second valuable metal leaching step (S32), after the first valuable metal leaching step (S31), ammonium persulfate ((NH4)2S2O8) is added secondarily in a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) can be leached secondarily.

[0049] In the third valuable metal leaching step (S31), after the second valuable metal leaching step (S32), ammonium persulfate ((NH4)2S2O8) is added for the third time at a set weight ratio, and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) can be leached for the third time.

[0050] Accordingly, copper can be recovered using ammonia water, and there is an advantage in that valuable metals such as Ni, Co, Mn, and Li can be selectively leached from the residue generated after copper recovery. In particular, according to various embodiments, the entire process can be carried out under distilled water and room temperature leaching. Accordingly, there are economic and environmentally friendly advantages.

[0051] Hereinafter, specific embodiments of a method for leaching valuable metals from spent lithium-ion batteries will be described.

[0052] [Example]

[0053] The waste lithium-ion batteries used in the present invention have a composition of the positive electrode active material content of the battery, with a ratio of Ni:Co:Mn ranging from 1:1:1 to 5:3:2, 6:2:2, and 8:1:1, and a mixture of two or more types of waste lithium-ion batteries was used.

[0054] In the leaching reaction, a 25–30 wt.% ammonia solution was used, and the additive ammonium persulfate ((NH4)2S2O8) was added in a ratio of 1:1 wt% to 4:1 wt.% relative to the sample. After leaching and recovering all of the copper, distilled water (H2O) was used as the leaching agent. [Table 1] below (see Fig. 4) shows the composition of the sample according to one embodiment, i.e., the black mass of the spent lithium-ion battery.

[0055] [Table 1]

[0056]

[0057] [Experimental Example of Copper Leaching Step]

[0058] Ammonia aqueous solutions were prepared using distilled water at concentrations of 25 vol.%, 50 vol.%, 75 vol.%, and 100 vol.%, and experiments were conducted under conditions of 45℃. The results are shown in [Table 2] (see Fig. 5).

[0059] [Table 2]

[0060]

[0061] Table 2 above shows the leaching rate of valuable metals, % (solid-liquid ratio: 0.5 / 10, 45℃, 150rpm) according to the concentration of ammonia water. Referring to Table 2, it can be seen that under the conditions of 100 vol.% ammonia water, 45℃, and 150rpm, all of copper (Cu) is leached, and 0.38% Co, 3.11% Ni, 0% Mn, and 19.54% Li are leached.

[0062] Copper (Cu) can be selectively leached from impurities such as iron (Fe) and aluminum (Al), and other valuable metals such as cobalt (Co), manganese (Mn), and nickel (Ni).

[0063] In addition, since lithium (Li) is not extracted in the solvent extraction process, which is a subsequent separation and purification process, lithium (Li) can be recovered as lithium carbonate from the solution remaining after all valuable metals have been recovered.

[0064] Meanwhile, [Table 3] below (see Fig. 6) shows the leaching rate of valuable metals using ammonia according to temperature, % (solid-liquid ratio: 0.5 / 10, 100 vol.% 150 rpm).

[0065] [Table 3]

[0066]

[0067] Referring to [Table 3], at a temperature of 100°C, the leaching rates of all valuable metals except lithium (Li) show a significantly decreasing trend. This is because the boiling point of ammonia is approximately 50°C, so at 100°C, most of the ammonia evaporates and does not affect the process of leaching valuable metals. [Equation 1] below represents the leaching reaction of valuable metals by ammonia.

[0068] Cu + 2NH4OH = Cu(NH4)2 + 2OH-

[0069] The reason the leaching rate of lithium (Li) increases with temperature is believed to be that lithium (Li) in the sample exists as a Li salt due to the electrolyte or the solid electrolyte interphase (SEI), and this is subsequently leached out.

[0070] [Experimental Example of Valuable Metal Leaching Step Using Ammonium Persulfate / Distilled Water]

[0071] An H2O-(NH4)2S2O8 leaching system was developed to reduce the discharge of leaching solution into hydrogen peroxide, the use of excessive acid, and energy consumption in the spent lithium-ion battery leaching process.

[0072] The H2O-(NH4)2S2O8 leaching system uses distilled water (H2O) as the leaching agent, and the entire leaching process takes place at room temperature. For this reason, it has the advantage of being more environmentally friendly than the conventional sulfuric acid-hydrogen peroxide reduction leaching process.

[0073] Tables 4, 5, and 6 below show the results according to the amount of ammonium persulfate ((NH4)2S2O8) added (see Figures 7 to 9).

[0074] [Table 4] below shows the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 1:1).

[0075] [Table 4]

[0076]

[0077] [Table 5] below shows the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 2:1).

[0078] [Table 5]

[0079]

[0080] [Table 6] below shows the leaching rate of valuable metals by the H2O-(NH4)2S2O8 system, % (leaching agent: distilled water, solid-liquid ratio: 0.5 / 10, temperature: room temperature, (NH4)2S2O8 input amount wt%: sample = 4:1).

[0081] [Table 6]

[0082]

[0083] Referring to the above [Tables 4], [Table 5], and [Table 6], it can be seen that the leaching rate of valuable metals is highest during the first leaching with ammonium persulfate ((NH4)2S2O8) input, and decreases significantly from the second leaching onwards. When leaching is performed up to a total of three times, it can be confirmed that the leaching rate of nickel (Ni) reaches approximately 90% when the amount of ammonium persulfate ((NH4)2S2O8) input is more than twice that of the sample. Additionally, it can be confirmed that the leaching rates of the remaining valuable metals, cobalt (Co), manganese (Mn), and lithium (Li), are less than 60% to 90%.

[0084] As described above, according to various embodiments of the present invention, copper can be recovered using ammonia water, and there is an advantage in that valuable metals such as Ni, Co, Mn, and Li can be selectively leached from the residue generated after copper recovery.

[0085] Furthermore, according to various embodiments of the present invention, all processes can be carried out under distilled water and room temperature leaching. Accordingly, there are economic and environmentally friendly advantages. The conventional process for leaching valuable metals from spent lithium-ion batteries is generally a sulfuric acid and hydrogen peroxide reduction leaching process. However, this process involves the use of excessive acid, energy consumption due to the atmospheric pressure heating leaching process, and the problem of solution ejection caused by the addition of hydrogen peroxide. Additionally, since impurities such as Fe and Al remain in the leaching solution after leaching, a precipitation process is required to remove them; in some cases, there is a trend to remove copper by considering it as an impurity rather than a recoverable material. According to various embodiments of the present invention, the aforementioned conventional problems are resolved, and there is an advantageous technical effect of selectively leaching valuable metals from spent lithium-ion batteries using a low-energy process that is more environmentally friendly than conventional methods.

[0086] Although the present invention has been described above with reference to the illustrated drawings, the present invention is not limited by the embodiments and drawings disclosed in this specification, and it is obvious that various modifications can be made by a person skilled in the art within the scope of the technical concept of the present invention. Furthermore, even if the effects of the configuration according to the present invention were not explicitly described while describing the embodiments of the present invention above, it is natural to acknowledge that the effects predictable by said configuration should also be recognized. Explanation of the symbols

[0087] S10: Waste Lithium-ion Battery Black Mass Preparation Phase S20: Selective copper leaching step using ammonia water S30: Valuable metal leaching step using ammonium persulfate / distilled water

Claims

Claim 1 The method comprises: a waste lithium-ion battery black mass preparation step (S10) for preparing waste lithium-ion battery black mass in powder form by undergoing a pretreatment process of crushing the waste lithium-ion battery; a copper leaching step (S20) for selectively leaching out and recovering all copper contained in the waste lithium-ion battery black mass using ammonia water having a set concentration and temperature; and a valuable metal leaching step (S30) using ammonium persulfate / distilled water for leaching out and recovering cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) by adding ammonium persulfate ((NH4)2S2O8) at a set weight ratio to the residue after the copper has been completely leached out, and using distilled water as a leaching agent. In the copper leaching step (S20), 100 vol.Using an ammonia solution at % and 45℃ with a stirring speed of 150 rpm, the copper contained in the spent lithium-ion battery black mass is entirely leached; in the valuable metal leaching step (S30) using ammonium persulfate / distilled water, the amount of ammonium persulfate ((NH4)2S2O8) added has a weight ratio of 2:1 or more relative to the sample; after passing through the valuable metal leaching step (S30) using ammonium persulfate / distilled water, nickel (Ni) has a leaching rate of at least 90%, while cobalt (Co), manganese (Mn), and lithium (Li) have a leaching rate of 60% to less than 90%; and in the valuable metal leaching step (S30) using ammonium persulfate / distilled water, ammonium persulfate ((NH4)2S2O8) is applied to the residue after the copper has been entirely leached at a set weight ratio A method for leaching valuable metals from a waste lithium-ion battery, comprising: a first valuable metal leaching step (S31) in which a first input is made and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached; a second valuable metal leaching step (S32) in which, after the first valuable metal leaching step (S31), ammonium persulfate ((NH4)2S2O8) is secondarily added at a set weight ratio and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached; and a third valuable metal leaching step (S33) in which, after the second valuable metal leaching step (S32), ammonium persulfate ((NH4)2S2O8) is thirdarily added at a set weight ratio and cobalt (Co), nickel (Ni), manganese (Mn), and lithium (Li) are leached. Claim 2 A method for leaching valuable metals from a waste lithium-ion battery according to claim 1, wherein in the waste lithium-ion battery black mass preparation step (S10), the waste lithium-ion battery is characterized by mixing at least two types of waste lithium-ion batteries among those in which the ratio of nickel (Ni):cobalt (Co):manganese (Mn), which is the composition of the positive electrode active material content of the battery, is 1:1:1, 5:3:2, 6:2:2, or 8:1:

1. Claim 3 delete Claim 4 A method for leaching valuable metals from waste lithium-ion batteries, further comprising, in claim 1, a step (S21) of recovering a copper solution by separating the leaching solution from solid to liquid after the copper leaching step (S20) in which the copper has been completely leached out. Claim 5 delete Claim 6 delete Claim 7 delete Claim 8 delete

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