WO2022161086A1 - Process for selectively recovering current collectors from spent lithium-ion batteries and application - Google Patents

Abstract

The present invention belongs to the technical field of the recycling of spent lithium-ion batteries, and provided is a process for selectively recovering current collectors from spent lithium-ion batteries, the process comprising the following steps: (1) discharging, drying, and incinerating the spent lithium-ion batteries, and then performing crushing, screening, and ball-milling to obtain a ball-milled material; (2) carrying out water washing and magnetic separation on the ball-milled material to obtain a low-magnetism current collector copper-aluminum mixture; and (3) pulping the low-magnetism current collector copper-aluminum mixture, and performing a shaking table treatment to obtain current collector copper and current collector aluminum, respectively. In the present invention, by ingeniously using the fact that the metals nickel, cobalt, and manganese have magnetic properties and copper and aluminum are non-magnetic, and the principle of the specific gravity of copper being significantly higher than that of aluminum, and by means of processes, such as a heat treatment, ball milling, hydraulic separation, a cyclone, magnetic separation, and a shaking table treatment, for the separation of copper and aluminum without new impurity ions being introduced throughout the separation process, the subsequent impurity removal process is greatly simplified, the purity of both the copper and aluminum current collectors are improved, and the sales value of the current collectors are improved.

Description

A process and application of selective recycling of waste lithium-ion battery to collect fluid technical field

The invention relates to the technical field of recycling waste lithium ion batteries, in particular to a process and application for selective recycling of waste lithium ion batteries to collect fluid.

Background technique

Li-ion batteries are widely used in various consumer electronic products, electric vehicles, energy storage and other fields due to their high voltage, high energy density, good cycle performance, low self-discharge, no memory effect, and wide operating temperature range. , With the increase in the number of lithium-ion batteries used, their subsequent reasonable recycling is an important issue that needs to be solved.

At present, the recovery methods of waste lithium-ion batteries mainly include acid leaching and roasting reduction. The acid leaching method is the most common treatment method at present. The waste is dissolved by acid leaching to dissolve the metal ions in the acid solution, and then the auxiliary materials are added to achieve selective leaching concentration. The purpose of fluid copper aluminum. The related art discloses a method for recovering copper powder from waste lithium batteries. The negative electrode material of the waste lithium battery is immersed in water, the carbon powder on the surface of the copper foil on the negative electrode material is peeled off and filtered, and then the copper foil is cleaned. To obtain clean copper foil; put the copper foil into a stainless steel plate and compact it, pass an oxidizing gas into the stainless steel plate containing the copper foil for oxidation treatment, and turn the material to obtain copper oxide powder; pass the copper oxide powder into The reducing gas is subjected to reduction treatment to obtain copper powder. The related art also discloses a method for separating a current collector and an active material of a lithium battery and its application. The method includes the following steps: S1. removing the electrode of the lithium battery; S2. immersing the electrode of the lithium battery at 75-85° C. In deionized water, anionic surfactant and hydrochloric acid are added at the same time, and the temperature is maintained and stirred for 4-6 hours to obtain reaction solution a; S3. Separation of current collector and active material. The related art also discloses a waste lithium battery recycling process, the method includes the following steps: step 1, the waste lithium battery is subjected to crushing treatment to obtain primary crushed materials; step 2, the primary crushed materials in step 1 are subjected to magnetic separation treatment, Magnetically select the iron in the primary crushed material, and obtain the iron-removed material; step 3, the iron-removed material in step 2 is deeply pulverized to obtain the deep-pulverized material; step 4, the deep-pulverized material in step 3 passes through the gravity separator Gravity separation is performed to obtain positive electrode material and negative electrode material respectively; in step 5, the positive electrode material in step 4 is subjected to airflow separation to obtain aluminum and positive electrode material; the negative electrode material is subjected to airflow separation to obtain copper and negative electrode material.

However, although the above method can achieve the purpose of selectively recovering and collecting fluid to a certain extent, there are also many shortcomings in the recovery process, such as complicated process, low purity of separated copper and aluminum, high cost, introduction of impurities or Harsh conditions. Therefore, it is of great significance in the art to develop a recovery process with simple operation, no pollution, and high purity of the recovered fluid.

SUMMARY OF THE INVENTION

The purpose of the present invention is to provide a process and application for selective recovery of waste lithium ion batteries to collect fluid, the process is simple to operate, realizes selective recovery of current collectors without introducing other impurities, and has good application prospects .

To achieve the above object, the present invention adopts the following technical solutions:

A process for selectively recovering a collection fluid from a spent lithium-ion battery, comprising the following steps:

(1) discharging the waste lithium-ion battery, drying, incinerating, and then performing crushing screening and ball milling to obtain the material after ball milling;

(2) get the material after described ball milling, through water washing and magnetic separation, obtain low magnetic current collector copper-aluminum mixture;

(3) The copper-aluminum mixture of the low-magnetic current collector is made into pulp, shaken, and the current collector copper and the current collector aluminum are obtained respectively.

Among them, the "low magnetic" of the copper-aluminum mixture of the low magnetic current collector means that there is little or no magnetic material. The prepared copper and aluminum current collectors can be directly sold.

Preferably, in step (1), the temperature of the incineration is 200-800° C., the heating method used in the incineration is constant-speed heating, and the heating rate is 5-50° C./min. The incineration treatment mainly heats the electrolyte in the waste lithium battery, which can crack the PVDF and CMC on the current collector, and strip off the precursor powder on the current collector, so as to achieve the purpose of recycling the collected fluid. The temperature of incineration is very important for this process. When the temperature is too low, PVDF and CMC are not fully cracked. When the temperature is too high, the current collector will be oxidized, reducing the sales value of the current collector.

More preferably, the heating rate is 10-20 °C/min. If the heating rate is too high, part of the current collector aluminum will be oxidized, and the lithium battery will be partially burned, resulting in low recovery purity of the current collector.

Preferably, in step (1), the discharge is to discharge the waste lithium-ion battery in a salt solution, and the salt solution includes at least one of sodium sulfate, magnesium sulfate, calcium sulfate, iron sulfate or potassium sulfate , More preferably, the salt solution is selected from sodium sulfate, and the cost of sodium sulfate is lower while ensuring the discharge efficiency.

Preferably, the mass concentration of the salt solution is 0.1-10%, and more preferably, the mass fraction of the salt solution is 0.1-1.0%.

Preferably, in step (1), the incineration treatment time is 30-300 min, more preferably 90-240 min.

Preferably, in step (1), the filling rate of the ball mill used in the ball milling is 0.1-0.4, more preferably 0.2-0.3.

Preferably, in step (1), the incineration treatment method is any one or a combination of two of incinerator calcination, (oxygen-free) cracking furnace calcination or electrolytic furnace calcination.

Preferably, in step (1), the waste lithium-ion battery is at least one of a polymer lithium battery, a soft-pack lithium battery, a power lithium battery or a non-liquid-injected battery cell.

Preferably, in step (2), the water washing process is as follows: the ball-milled material is first washed with a rotary drum hydraulic sieve, and then the first washed material is washed with a cyclone for a second time. The rotary drum hydraulic sieve mainly separates the copper-aluminum current collector and the battery powder; the cyclone is used for the second washing of the current collector, and the battery powder remaining on the copper-aluminum current collector is washed, thereby further reducing the amount of the copper-aluminum current collector. Sticky battery powder and other impurities.

Preferably, in step (2), the magnetic field strength of the magnetic separator is 3000Gs～20000Gs, more preferably 5000Gs～10000Gs.

Preferably, in step (2), the particle size of the low magnetic current collector copper-aluminum mixture is 2-80 mesh, more preferably 20-60 mesh.

Preferably, in step (3), the liquid-solid volume ratio of the slurry is (0.5-10):1, more preferably (1-5):1.

Preferably, in step (3), before the pulping, the process of screening the low-magnetic current collector copper-aluminum mixture is also included, and the undersize is taken for pulping, and the mesh size of the screen is 40-60 mesh; more preferably 60 mesh. The screening process can stratify the materials, which is beneficial to the subsequent shaking table sorting.

Preferably, in step (3), the sieved large particles on the sieve are crushed again by a fine crusher, and then the current collector copper and the current collector aluminum are separated by a shaker.

Preferably, in step (3), the lateral inclination angle of the shaking table is 0-10°, more preferably 1-5°. Appropriate inclination angle can increase the transverse shear force of the material, reduce the friction force of the material on the shaking table surface, so that the material can move in the direction of the water flow; increasing the transverse inclination angle can make the material diffuse and stratify rapidly, so as to achieve the best separation efficiency. Purpose.

Preferably, in step (2), the low magnetic current collector copper-aluminum mixture is a copper-aluminum mixture of a one-element lithium battery, a copper-aluminum mixture of a ternary lithium battery, a copper-aluminum mixture of a steel-shell lithium battery, or a copper-aluminum mixture of a power lithium battery. at least one.

The invention also provides an application of the process in recycling waste lithium ion batteries.

Advantages of the present invention:

The invention cleverly utilizes the principle that nickel, cobalt and manganese metals are magnetic, copper and aluminum are non-magnetic, and the specific gravity of copper is obviously higher than that of aluminum. The process of sorting copper and aluminum does not introduce new impurity ions in the whole separation process, which greatly simplifies the subsequent impurity removal process and improves the purity of copper and aluminum current collectors. The purity of copper current collectors can reach 98%, and the purity of aluminum current collectors It can reach 85%, which improves the sales value of the current collector and has a good application prospect.

Description of drawings

The above and/or additional aspects and advantages of the present invention will become apparent and readily understood from the following description of embodiments taken in conjunction with the accompanying drawings, wherein:

1 is a process flow diagram of Embodiment 1 of the present invention;

Fig. 2 is the process flow diagram of the comparative example of the present invention.

Detailed ways

In order to have an in-depth understanding of the present invention, the preferred experimental scheme of the present invention is described below in conjunction with examples to further illustrate the features and advantages of the present invention. The protection scope of the invention is determined by the scope of the appended claims.

Example 1

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble and soak the waste polymer lithium battery in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 500 ℃ ℃, the time is 90min, the heating rate is 10℃/min, the battery after drying and incineration heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh sieve, and the material on the sieve is ball-milled to obtain material after ball milling;

(2) The ball-milled material is first washed with a rotary drum hydraulic sieve, and the first washed material is washed with a second water by a cyclone to obtain a slurry and a collector with magnetic materials, and the magnetic materials are washed with water for a second time. After the current collector is processed by a magnetic separator, a low magnetic current collector copper-aluminum mixture is obtained;

(3) Take the low magnetic current collector copper-aluminum mixture and sieve it with 60 meshes, take the material under the sieve, mix it with water at a liquid-solid volume ratio of 1:1, and pass through the shaker for sorting, and the horizontal inclination angle of the shaker sorting is 1°. After sorting, the current collector copper and the current collector aluminum are obtained, and the large particles on the screen are broken again by the fine crusher, and then the current collector copper and the current collector aluminum are separated by the shaking table.

The copper-aluminum mixture after passing through the 60-mesh sieve in step (3) of the present embodiment and the current collector after the shaker separation are detected, and the inductively coupled plasma emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer are used to detect and detect. The results are shown in Table 1. The calculated purity of the current collector copper is 96.31%, and the purity of the current collector aluminum is 82.06%. The current collectors sorted by the shaker can be sold directly.

Table 1 embodiment 1 metal element content and product detection result

element Cu Al Ni Co Mn 60 mesh undersize (%) 58.31 22.35 0.90 0.69 0.17 Sorted current collector Cu (%) 96.31 2.03 0.10 0.11 0 Sorted current collector Al (%) 2.32 82.06 0.17 0.12 0.03

Fig. 1 is the process flow diagram of the embodiment of the present invention 1, as can be seen from Fig. 1, the waste lithium battery obtains the larger particle size oversize and smaller particle size undersize after drying, burning, crushing and sieving , the material under the sieve is black powder, and the material on the sieve is ball milled, then washed by a rotary drum hydraulic sieve and a cyclone in turn, to remove materials with smaller particle size such as black powder remaining on the current collector, and the washed material passes through Magnetic separation removes magnetic materials such as steel shells, then sieves to obtain particles with smaller particle sizes, and finally uses a shaker to separate current collector copper and current collector aluminum. The process steps are simple and environmentally friendly.

Example 2

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble and soak the waste polymer lithium battery in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 500 ℃ ℃, the time is 180min, the heating rate is 20℃/min, the battery after drying, incineration and heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh sieve, and the material on the sieve is ball-milled to obtain material after ball milling;

(2) The ball-milled material is first washed with a rotary drum hydraulic sieve, and the first washed material is washed with a second water by a cyclone to obtain a slurry and a collector with magnetic materials, and the magnetic materials are washed with water for a second time. After the current collector is processed by a magnetic separator, a low magnetic current collector copper-aluminum mixture is obtained;

(3) Take the low magnetic current collector copper-aluminum mixture and sieve it with 60 meshes, take the under-sieve, mix it with water at a liquid-solid volume ratio of 1:1, and pass through the shaker sorting, and the shaker sorting lateral inclination angle is 2° After sorting, the current collector copper and the current collector aluminum are obtained, and the large particles on the screen are broken again by the fine crusher, and then the current collector copper and the current collector aluminum are separated by the shaking table.

The copper-aluminum mixture after passing through the 60-mesh sieve in step (3) of the present embodiment and the current collector after the shaker separation are detected, and the inductively coupled plasma emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer are used to detect and detect. The results are shown in Table 2. The calculated purity of the current collector copper is 95.89%, and the purity of the current collector aluminum is 81.32%. The current collectors sorted by the shaker can be sold directly.

Table 2 embodiment 2 metal element content and product detection result

element Cu Al Ni Co Mn

60 mesh undersize (%) 60.28 23.24 0.81 0.63 0.12 Sorted current collector Cu (%) 95.89 1.23 0.04 0.06 0 Sorted current collector Al (%) 1.32 81.32 0.05 0.07 0.02

Example 3

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble the waste polymer lithium battery and soak it in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 600 ℃ ℃, the time is 90min, the heating rate is 20℃/min, the battery after drying and incineration heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh sieve, and the material on the sieve is taken for ball milling to obtain material after ball milling;

(2) The ball-milled material is first washed with a rotary drum hydraulic sieve, and the first washed material is washed with a second water by a cyclone to obtain a slurry and a collector with magnetic materials, and the magnetic materials are washed with water for a second time. After the current collector is processed by a magnetic separator, a low magnetic current collector copper-aluminum mixture is obtained;

(3) Take the low magnetic current collector copper-aluminum mixture and sieve it with 40 meshes, take the under-sieve, mix it with water at a liquid-solid volume ratio of 2:1, and pass through the shaker sorting, and the shaker sorting lateral inclination angle is 2° After sorting, the current collector copper and the current collector aluminum are obtained, and the large particles on the screen are broken again by the fine crusher, and then the current collector copper and the current collector aluminum are separated by the shaking table.

The copper-aluminum mixture after passing through the 40-mesh sieve in the step (3) of the present embodiment and the current collector after the shaker separation are detected, and the inductively coupled plasma emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer are used to detect, detect The results are shown in Table 3. The calculated purity of the current collector copper is 96.74%, and the purity of the current collector aluminum is 82.56%. The current collectors sorted by the shaker can be sold directly.

Table 3 embodiment 3 metal element content and product detection result

element Cu Al Ni Co Mn 40 mesh undersize (%) 63.32 27.21 0.49 0.44 0.08 Sorted current collector Cu (%) 96.74 0.61 0.03 0.05 0 Sorted current collector Al (%) 0.87 82.56 0.04 0.07 0.03

Example 4

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble and soak the waste polymer lithium battery in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 500 ℃ ℃, the time is 90min, the heating rate is 10℃/min, the battery after drying and incineration heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh sieve, and the material on the sieve is ball-milled to obtain material after ball milling;

(2) The ball-milled material is first washed with a rotary drum hydraulic sieve, and the first washed material is washed with a second water by a cyclone to obtain a slurry and a collector with magnetic materials, and the magnetic materials are washed with water for a second time. After the current collector is processed by a magnetic separator, a low magnetic current collector copper-aluminum mixture is obtained;

(3) Take the low magnetic current collector copper-aluminum mixture and sieve it with 40 meshes, take the material under the sieve, mix it with water at a liquid-solid volume ratio of 1:1, and pass through the shaker for sorting, and the horizontal inclination angle of the shaker sorting is 2°. After sorting, the current collector copper and the current collector aluminum are obtained, and the large particles on the screen are broken again by the fine crusher, and then the current collector copper and the current collector aluminum are separated by the shaking table.

The copper-aluminum mixture after passing through the 40-mesh sieve in the step (3) of the present embodiment and the current collector after the shaker separation are detected, and the inductively coupled plasma emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer are used to detect, detect The results are shown in Table 4. The calculated purity of the current collector copper is 97.89%, and the purity of the current collector aluminum is 85.07%. The current collectors sorted by the shaker can be sold directly.

Table 4 embodiment 4 metal element content and product detection result

element Cu Al Ni Co Mn 40 mesh undersize (%) 64.40 30.30 0.60 0.51 0.10 Sorted current collector Cu (%) 97.89 0.52 0.03 0.04 0 Sorted current collector Al (%) 0.69 85.07 0.04 0.06 0.02

Example 5

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble and soak the waste polymer lithium battery in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 500 ℃ ℃, the time is 90min, the heating rate is 10℃/min, the battery after drying and incineration heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh sieve, and the material on the sieve is ball-milled to obtain material after ball milling;

(2) The ball-milled material is first washed with a rotary drum hydraulic sieve, and the first washed material is washed with a second water by a cyclone to obtain a slurry and a collector with magnetic materials, and the magnetic materials are washed with water for a second time. After the current collector is processed by a magnetic separator, a low magnetic current collector copper-aluminum mixture is obtained;

(3) Take the low magnetic current collector copper-aluminum mixture and sieve it with 40 meshes, take the under-sieve, mix it with water at a liquid-solid volume ratio of 2:1, and pass through the shaker sorting, and the shaker sorting lateral inclination angle is 3° After sorting, the current collector copper and the current collector aluminum are obtained, and the large particles on the screen are broken again by the fine crusher, and then the current collector copper and the current collector aluminum are separated by the shaking table.

The copper-aluminum mixture after passing through the 40-mesh sieve in the step (3) of the present embodiment and the current collector after the shaker separation are detected, and are detected by inductively coupled plasma emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer. The results are shown in Table 5. The calculated purity of the current collector copper is 95.87%, and the purity of the current collector aluminum is 82.01%. The current collectors sorted by the shaker can be sold directly.

Table 5 embodiment 5 metal element content and product detection result

element Cu Al Ni Co Mn 40 mesh undersize (%) 64.40 30.30 0.60 0.51 0.10 Sorted current collector Cu (%) 95.87 1.03 0.08 0.07 0.01 Sorted current collector Al (%) 1.23 82.01 0.11 0.10 0.03

Comparative ratio

A method for selectively recovering a collection fluid from a lithium polymer battery, comprising the steps of:

(1) Disassemble and soak the waste polymer lithium battery in sodium sulfate solution for discharge treatment, when discharged to a voltage less than 0.5V, remove it, put it into an incinerator for drying and incineration heat treatment, and set the heat treatment temperature to be 500 ℃ ℃, the time is 90min, the heating rate is 10℃/min, the battery after drying and incineration heat treatment is crushed with a crusher, the crushed material is sieved through a 60-mesh screen, and the material on the screen is crushed for the second time Screening to obtain the second crushed and screened material;

(2) The materials after the second crushing and screening are separated by air flow to obtain the current collector copper and the current collector aluminum respectively.

The current collectors obtained by air separation in step (2) of this comparative example were detected by inductively coupled plasma optical emission spectroscopy (ICP-OES) and atomic absorption spectrophotometer. The detection results are shown in Table 6. The calculated average purity of copper in the current collector is 80.11%, (n=3), and the average purity of aluminum in the current collector is 69.50%, (n=3).

Table 6 Comparative example metal element content and product detection results

Comparative Examples 1 to 5, the traditional process comparative example process has two shortcomings:

1. Comparative Examples 1 to 5, adopt the traditional fire process comparative example to carry out sorting, there is a lot of dust in the sorting process, which not only damages the health of people and causes heavy metal poisoning, but also the production environment is not easy to control.

2. Comparative Examples 1 to 5 analyze and detect the results, and the collectors obtained by the traditional process example have low purity and high impurity content. The use of the comparative process not only reduces the economic value of the current collectors copper and aluminum, but also reduces the recovery rate of precious metals (Ni, Co, Mn).

Fig. 2 is the process flow diagram of the comparative example of the present invention, as can be seen from Fig. 2, after the waste lithium battery is dried, incinerated, crushed and sieved to obtain larger particle size oversize and smaller particle size undersize, The material under the sieve is black powder, and the material on the sieve is crushed and sieved for the second time, and the current collector copper and aluminum are obtained by air separation. The whole process adopts the fire separation process, which not only causes serious environmental pollution, but also reduces the economic value of the collector copper and aluminum and the recovery and recycling value of precious metals.

The process and application of the selective recovery of waste lithium-ion batteries provided by the present invention and the application of the fluid collection have been introduced in detail above. The principles and implementations of the present invention are described with specific examples in this paper. The descriptions of the above examples are only used for To aid in understanding the methods of the invention and their core concepts, including the best mode, and also to enable any person skilled in the art to practice the invention, including making and using any devices or systems, and performing any incorporated methods. It should be pointed out that for those skilled in the art, without departing from the principle of the present invention, several improvements and modifications can also be made to the present invention, and these improvements and modifications also fall within the protection scope of the claims of the present invention. The scope of patent protection of the present invention is defined by the claims, and may include other examples that occur to those skilled in the art. Such other embodiments are intended to be within the scope of the claims if they have structural elements that do not differ from the literal language of the claims, or if they include equivalent structural elements with insubstantial differences from the literal language of the claims.

Claims (10)

A process for selective recovery of waste lithium-ion batteries to collect fluid, comprising the following steps: (1) discharging the waste lithium-ion battery, drying, incinerating, and then performing crushing screening and ball milling to obtain the material after ball milling; (2) get the material after described ball milling, through water washing and magnetic separation, obtain low magnetic current collector copper-aluminum mixture; (3) The copper-aluminum mixture of the low-magnetic current collector is made into pulp, shaken, and the current collector copper and the current collector aluminum are obtained respectively. technology according to claim 1, is characterized in that, in step (1), the temperature of described incineration is 200～800 ℃, the heating mode that incineration adopts is constant speed heating up, and the rate of heating is 5～50 ℃/min . The process according to claim 1, characterized in that, in step (1), the discharge is to discharge the waste lithium-ion battery in a salt solution, and the salt solution comprises sodium sulfate, magnesium sulfate, calcium sulfate, At least one of ferric sulfate or potassium sulfate; the mass concentration of the salt solution is 0.1-10%. The process according to claim 1, characterized in that, in step (1), the burning time is 30-300 min. The process according to claim 1, characterized in that, in step (1), the filling rate of the ball mill used in the ball milling is 0.1-0.4. The process according to claim 1, characterized in that, in step (2), the washing process is as follows: the ball-milled material is first washed with a rotary drum hydraulic sieve, and then the washed material is passed through a swirling flow The device is washed for the second time. The process according to claim 1, characterized in that, in step (3), before the pulping, it further comprises a process of screening the low-magnetic current collector copper-aluminum mixture, and taking the undersize for pulping , the mesh number of the screen is 40-60 mesh. The process according to claim 1, wherein in step (3), the liquid-solid volume ratio of the slurry is (0.5-10):1. The process according to claim 1, wherein in step (3), the lateral inclination angle of the shaking table is 0-10°. Application of the process described in any one of claims 1-9 in recycling spent lithium-ion batteries.

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