CN112467224A - Electrochemical uniform lithium pre-preparing method for lithium ion battery - Google Patents
Electrochemical uniform lithium pre-preparing method for lithium ion battery Download PDFInfo
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- CN112467224A CN112467224A CN202011144713.7A CN202011144713A CN112467224A CN 112467224 A CN112467224 A CN 112467224A CN 202011144713 A CN202011144713 A CN 202011144713A CN 112467224 A CN112467224 A CN 112467224A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract
The invention discloses an electrochemical uniform pre-lithium method of a lithium ion battery, which relates to the technical field of lithium ion batteries and comprises the following steps: alternately stacking a positive plate and a negative plate on one side of the copper-lithium composite layer from inside to outside according to a stacking mode to form an upper electric core unit; similarly, alternately stacking a negative plate and a positive plate on the other side of the copper-lithium composite layer to form a lower electric core unit; diaphragms are arranged between the positive plate and the negative plate, between the upper battery cell unit and the copper-lithium composite layer and between the lower battery cell unit and the copper-lithium composite layer; the copper-lithium composite layer comprises a copper foil and metal lithium layers coated on the upper surface and the lower surface of the copper foil; injecting electrolyte into the battery to carry out pre-lithiation treatment; and after the pre-lithiation is finished, taking out the diaphragm between the copper-lithium composite layer and the upper battery cell unit or the lower battery cell unit, and finally sealing the battery. The current collector adopts a perforated structure, so that lithium is more uniformly embedded, and the lithium pre-preparation is simple and easy to operate.
Description
Technical Field
The invention relates to the technical field of lithium ion batteries, in particular to an electrochemical uniform lithium pre-preparing method of a lithium ion battery.
Background
In the first charge and discharge process of the lithium ion battery, due to structural change or the formation of a surface SEI film, part of active lithium is consumed, and the capacity of the battery is reduced. The loss of capacity of the negative electrode can be improved by pre-intercalation of lithium. Currently, commonly used methods for pre-embedding lithium include lithium foil lithium supplement, metal lithium powder coating, lithium salt solution electrolysis and the like. The control difficulty of lithium supplement of the lithium foil is high, the requirement on the use environment of the metal lithium powder is high, and the lithium supplement step of the electrolytic lithium salt solution is complicated.
Disclosure of Invention
Based on the technical problems in the background art, the invention provides an electrochemical uniform lithium pre-preparing method for a lithium ion battery, which is uniform in lithium intercalation, simple and easy to operate.
The invention provides an electrochemical uniform pre-lithium method of a lithium ion battery, which comprises the following steps:
s1, alternately stacking a positive plate and a negative plate from inside to outside on one side of the copper-lithium composite layer according to a stacking mode to form an upper battery cell, and alternately stacking the negative plate and the positive plate from inside to outside on the other side of the copper-lithium composite layer according to the stacking mode to form a lower battery cell; the number of the positive plates or the negative plates in the upper cell unit and the lower cell unit is equal, and diaphragms are arranged between the positive plates and the negative plates, between the upper cell unit and the copper-lithium composite layer and between the lower cell unit and the copper-lithium composite layer; the copper-lithium composite layer comprises a copper foil and metal lithium layers coated on the upper surface and the lower surface of the copper foil;
s2, preparing a laminated battery according to the assembly sequence of the upper battery cell unit, the copper-lithium composite layer and the lower battery cell unit, injecting electrolyte into the battery, and respectively connecting the copper-lithium composite layer and the negative plate with a charge-discharge test cabinet to perform pre-lithiation treatment;
and S3, after the pre-lithiation is finished, taking out the diaphragm between the copper-lithium composite layer and the upper cell unit or the lower cell unit, and finally sealing the battery to finish the pre-lithiation of the battery.
In the invention S1, the area of the lithium metal layer is equal to or slightly larger than the area of the negative electrode material on the negative electrode sheet.
In the present invention S1, a tab is provided on the copper foil of the copper-lithium composite layer on a surface perpendicular to the positive and negative electrode tab sides.
Preferably, the positive plate comprises a positive current collector and a positive active material, the positive current collector is a perforated aluminum foil or a perforated polymer metal aluminum laminated composite foil, and the preferred thickness is 8-15 μm; preferably, the positive electrode active material includes one of lithium cobaltate, lithium iron phosphate, and a ternary positive electrode material.
Preferably, the negative plate comprises a negative current collector and a negative active material, the negative current collector is a perforated copper foil or a perforated polymer metal copper laminated composite foil, and the preferred thickness is 6-12 μm; preferably, the negative active material includes one of graphite, a silicon-carbon composite material, silicon monoxide, and nanocrystalline silicon.
Preferably, in S2, the negative plate is connected with the positive electrode of the charge-discharge test cabinet, the copper-lithium composite layer is connected with the negative electrode of the charge-discharge test cabinet for pre-lithiation treatment, the cut-off voltage is 0.01-2.5V, and the discharge current is 0.02-0.5C; preferably, the temperature of the pre-lithiation treatment is 25-50 ℃.
Preferably, the prelithiation treatment comprises a constant current discharge and a standing step; the constant current discharge time t is C multiplied by a/I, wherein C is the capacity of the negative electrode, a is the percentage of the capacity of the pre-embedded lithium to the capacity of the negative electrode, and I is the discharge current; preferably, the standing time is 8-48 h.
Preferably, in the prelithiation treatment, the mass M of the prelithiation is (M × C × a × 3600)/F, where M is the molar mass of lithium, F is the faraday constant, C is the capacity of the negative electrode, and a is the percentage of the capacity of the prelithiation to the capacity of the negative electrode.
In the present invention, the amount of metallic lithium is equal to or slightly more than the amount of pre-intercalated lithium.
Preferably, the total thickness of the double-sided metallic lithium layers is > m/(ρ A), ρ is the density of the metallic lithium, and A is the surface area of the metallic lithium layer.
Preferably, in the copper-lithium composite layer, the thickness of the copper foil is 4-15 μm.
Has the advantages that: the pre-lithium method provided by the invention can effectively improve the capacity and the first effect of the battery, is simple and easy to operate, has low requirement on the environment, and improves the uniformity of the pre-lithium on the premise of not influencing the performance of the battery due to the introduced perforated current collector.
Drawings
Fig. 1 is an internal sectional view of a battery of the present invention;
fig. 2 is an external view of the battery of the present invention.
Detailed Description
According to the battery adopted by the invention, the positive electrode active material comprises one of lithium cobaltate, lithium iron phosphate and a ternary positive electrode material, the current collector is a perforated aluminum foil or a perforated polymer metal aluminum laminated composite foil, and the thickness of the current collector is 8-15 mu m; the negative active material comprises one of graphite, a silicon-carbon composite material, silicon monoxide and nanocrystalline silicon, and the current collector is a perforated copper foil or a perforated polymer metal copper laminated composite material, and the thickness of the current collector is 6-12 mu m.
The copper-lithium composite layer has the structure as follows: the metal lithium is positioned on two sides of the copper foil to form a metal lithium/copper foil/metal lithium layered structure, and one side of the copper foil is provided with a tab. The thickness of the metallic lithium is determined according to the content of the negative electrode active material and the negative electrode pre-intercalation capacity, and the amount of the metallic lithium is equal to or slightly more than the amount of the remaining pre-intercalation. The thickness of the copper foil is between 4 and 15 μm. The area of the lithium layer is the same as or slightly higher than that of the cathode material.
The pre-lithium amount was calculated as follows: m is (M × C × a × 3600)/F, M is the mass of pre-intercalation lithium in g, M is the molar mass of lithium, F is the faraday constant, C is the capacity of the negative electrode, and a is the percentage of the pre-intercalation lithium capacity to the negative electrode capacity, and is generally 5 to 50%. The thickness of the lithium metal layer is slightly higher than m/(rho A), rho is the density of the lithium metal, and A is the surface area of the lithium layer.
As shown in fig. 1, in the present invention, a copper-lithium composite layer is inserted into the center of the battery, positive and negative plates are alternately stacked in a stacked manner on one side of the copper-lithium composite layer, and negative and positive plates are stacked in a stacked manner on the other side of the copper-lithium composite layer. The negative plate and the positive plate, and the pole plate and the lithium metal are separated by a diaphragm.
As shown in fig. 2, the battery is packaged into an aluminum-plastic film, wherein the positive and negative electrode tabs are positioned on the same side or opposite sides of the battery, the copper-lithium composite layer tab is positioned on one side perpendicular to the positive and negative electrode tabs, the aluminum-plastic film on one side of the copper-lithium composite layer tab is not sealed, and after heat sealing of the other three sides, electrolyte is injected. Pre-embedding lithium into the battery, and in the pre-lithiation process, respectively connecting a lug and a negative lug of a copper-lithium composite layer with a charge-discharge test cabinet to discharge metal lithium to a negative active material, wherein the discharge current is 0.02C-0.5C, the pre-lithiation time t of the battery is cxa/I, I is the discharge current, the unit of t is h, and the temperature in the whole process is 25-50 ℃.
And after the pre-lithium is finished, taking out the copper-lithium composite layer and the diaphragm on one side of the copper-lithium composite layer, keeping the diaphragm on the other side of the copper-lithium composite layer, sealing the battery, and standing for 8-48 hours.
Example 1
The embodiment provides a lithium pre-intercalation method for a lithium ion battery, which comprises the following specific operation processes:
in the battery adopted in this embodiment, the positive electrode active material is lithium iron phosphate, the current collector is a perforated aluminum foil, the thickness of the current collector is 12 μm, the negative electrode active material is a silicon-carbon composite material, and the current collector is a perforated copper foil, the thickness of the current collector is 8 μm. The battery size was 10014010(mm), and the design capacity was 10 Ah.
The thickness of the copper-lithium composite layer copper foil in this example was 10 μm. The area of the lithium layer is the same as the negative electrode. The cell had a pre-lithium insertion of 8% and a single-sided lithium layer thickness of 18 μm.
In this embodiment, a copper-lithium composite layer is inserted into the center of the battery, 8 positive plates and 8 negative plates are sequentially and alternately stacked on one side of the copper-lithium composite layer in a stacking manner, and 8 negative plates and 7 positive plates are sequentially stacked on the other side of the copper-lithium composite layer in a stacking manner. The negative plate and the positive plate, and the pole plate and the lithium metal are separated by a diaphragm.
The battery is arranged in an aluminum plastic film, wherein the positions of positive and negative electrode lugs are arranged on the same side or the opposite side of the battery, the position of the lug of the copper-lithium composite layer is arranged on one side vertical to the positive and negative electrode lugs, the aluminum plastic film on one side of the lug of the copper-lithium composite layer is not sealed, and electrolyte is injected after the other three sides are subjected to heat sealing. Pre-embedding lithium into the battery, and in the pre-lithiation process, respectively connecting a tab and a negative tab on a copper foil of a copper-lithium composite layer with a charge-discharge test cabinet to discharge metal lithium to the silicon-carbon composite material, wherein the discharge current is 0.05A, the pre-lithiation time of the battery is 16h, and the temperature in the whole process is 45 ℃.
And after the pre-lithium is finished, taking out the copper-lithium composite layer and the diaphragm on one side of the copper-lithium composite layer, reserving the diaphragm on the other side of the copper-lithium composite layer, sealing the battery, and standing for 48 hours at 45 ℃.
Example 2
The embodiment provides a lithium pre-intercalation method for a lithium ion battery, which comprises the following specific operation processes:
in the battery adopted in this embodiment, the positive electrode active material is ternary NCM811, the current collector is a perforated aluminum foil with a thickness of 12 μm, the negative electrode active material is a silicon-carbon composite material, and the current collector is a perforated copper foil with a thickness of 8 μm. The battery size was 10014010(mm), and the design capacity was 10 Ah.
The thickness of the copper-lithium composite layer copper foil in this example was 10 μm. The area of the lithium layer is the same as the negative electrode. The cell had a pre-lithium insertion of 10% and a single-sided lithium layer thickness of 23 μm.
In this embodiment, a copper-lithium composite layer is inserted into the center of the battery, 8 positive plates and 8 negative plates are sequentially and alternately stacked on one side of the copper-lithium composite layer in a stacking manner, and 8 negative plates and 7 positive plates are sequentially stacked on the other side of the copper-lithium composite layer in a stacking manner. The negative plate and the positive plate, and the pole plate and the lithium metal are separated by a diaphragm.
The battery is arranged in an aluminum plastic film, wherein the positions of positive and negative electrode lugs are arranged on the same side or the opposite side of the battery, the position of the lug of the copper-lithium composite layer is arranged on one side vertical to the positive and negative electrode lugs, the aluminum plastic film on one side of the lug of the copper-lithium composite layer is not sealed, and electrolyte is injected after the other three sides are subjected to heat sealing. Pre-embedding lithium into the battery, and in the pre-lithiation process, respectively connecting a tab and a negative tab on a copper foil of a copper-lithium composite layer with a charge-discharge test cabinet to discharge metal lithium to the silicon-carbon composite material, wherein the discharge current is 0.05A, the pre-lithiation time of the battery is 20 hours, and the temperature in the whole process is 45 ℃.
And after the pre-lithium is finished, taking out the copper-lithium composite layer and the diaphragm on one side of the copper-lithium composite layer, reserving the diaphragm on the other side of the copper-lithium composite layer, sealing the battery, and standing for 48 hours at 45 ℃.
Example 3
The embodiment provides a lithium pre-intercalation method for a lithium ion battery, which comprises the following specific operation processes:
in the battery adopted in this embodiment, the positive electrode active material is lithium iron phosphate, the current collector is a perforated aluminum foil, the thickness of the current collector is 12 μm, the negative electrode active material is graphite, and the current collector is a perforated copper foil, the thickness of the current collector is 8 μm. The battery size was 10014010(mm), and the design capacity was 10 Ah.
The thickness of the copper-lithium composite layer copper foil in this example was 10 μm. The area of the lithium layer is the same as the negative electrode. The pre-lithium insertion of the cell was 5% and the thickness of the single-sided lithium layer was 12 μm.
In this embodiment, a copper-lithium composite layer is inserted into the center of the battery, 8 positive plates and 8 negative plates are sequentially and alternately stacked on one side of the copper-lithium composite layer in a stacking manner, and 8 negative plates and 7 positive plates are sequentially stacked on the other side of the copper-lithium composite layer in a stacking manner. The negative plate and the positive plate, and the pole plate and the lithium metal are separated by a diaphragm.
The battery is arranged in an aluminum plastic film, wherein the positions of positive and negative electrode lugs are arranged on the same side or the opposite side of the battery, the position of the lug of the copper-lithium composite layer is arranged on one side vertical to the positive and negative electrode lugs, the aluminum plastic film on one side of the lug of the copper-lithium composite layer is not sealed, and electrolyte is injected after the other three sides are subjected to heat sealing. Pre-embedding lithium into the battery, and in the pre-lithiation process, respectively connecting a tab and a negative tab on a copper foil of a copper-lithium composite layer with a charge-discharge test cabinet to discharge metal lithium to graphite, wherein the discharge current is 0.05A, the pre-lithiation time of the battery is 10 hours, and the temperature in the whole process is 45 ℃.
And after the pre-lithium is finished, taking out the copper-lithium composite layer and the diaphragm on one side of the copper-lithium composite layer, reserving the diaphragm on the other side of the copper-lithium composite layer, sealing the battery, and standing for 48 hours at 45 ℃.
The batteries produced in the same batch in examples 1-3 were divided into 2 groups, one group was designated as a reference battery without pre-lithiation treatment, the other group was designated as a pre-lithium battery with pre-lithiation treatment, and the two groups were subjected to chemical composition and capacity grading, the first effects of which are shown in table 1.
TABLE 1 first Effect data for pre-lithiated batteries of examples 1-3
As can be seen from table 1, the first efficiency of the pre-lithiated battery is significantly improved compared to the reference battery.
The above description is only for the preferred embodiment of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art should be considered to be within the technical scope of the present invention, and the technical solutions and the inventive concepts thereof according to the present invention should be equivalent or changed within the scope of the present invention.
Claims (8)
1. An electrochemical uniform pre-lithium method of a lithium ion battery is characterized by comprising the following steps:
s1, alternately stacking a positive plate and a negative plate from inside to outside on one side of the copper-lithium composite layer according to a stacking mode to form an upper battery cell, and alternately stacking the negative plate and the positive plate from inside to outside on the other side of the copper-lithium composite layer according to the stacking mode to form a lower battery cell; the number of the positive plates or the negative plates in the upper cell unit and the lower cell unit is equal, and diaphragms are arranged between the positive plates and the negative plates, between the upper cell unit and the copper-lithium composite layer and between the lower cell unit and the copper-lithium composite layer; the copper-lithium composite layer comprises a copper foil and metal lithium layers coated on the upper surface and the lower surface of the copper foil;
s2, preparing a laminated battery according to the assembly sequence of the upper battery cell unit, the copper-lithium composite layer and the lower battery cell unit, injecting electrolyte into the battery, and respectively connecting the copper-lithium composite layer and the negative plate with a charge-discharge test cabinet to perform pre-lithiation treatment;
and S3, after the pre-lithiation is finished, taking out the diaphragm between the copper-lithium composite layer and the upper cell unit or the lower cell unit, and finally sealing the battery to finish the pre-lithiation of the battery.
2. The electrochemical uniform pre-lithium method for the lithium ion battery according to claim 1, wherein the positive plate comprises a positive current collector and a positive active material, the positive current collector is a perforated aluminum foil or a perforated polymer metal aluminum laminated composite foil, and the preferred thickness is 8-15 μm; preferably, the positive electrode active material includes one of lithium cobaltate, lithium iron phosphate, and a ternary positive electrode material.
3. The electrochemical uniform pre-lithium method of the lithium ion battery according to claim 1 or 2, characterized in that the negative plate comprises a negative current collector and a negative active material, the negative current collector is a perforated copper foil or a perforated polymer metal copper laminated composite foil, and the thickness is preferably 6-12 μm; preferably, the negative active material includes one of graphite, a silicon-carbon composite material, silicon monoxide, and nanocrystalline silicon.
4. The electrochemical uniform pre-lithium method of the lithium ion battery according to any one of claims 1 to 3, characterized in that in S2, the negative plate is connected with the positive electrode of the charge-discharge test cabinet, the copper-lithium composite layer is connected with the negative electrode of the charge-discharge test cabinet for pre-lithium treatment, the cut-off voltage is 0.01 to 2.5V, and the discharge current is 0.02 to 0.5C; preferably, the temperature of the pre-lithiation treatment is 25-50 ℃.
5. The electrochemical homogeneous pre-lithiation process for lithium ion batteries according to any one of claims 1 to 4, characterized in that said pre-lithiation treatment comprises a constant current discharge and a resting step; the constant current discharge time t is C multiplied by a/I, wherein C is the capacity of the negative electrode, a is the percentage of the capacity of the pre-embedded lithium to the capacity of the negative electrode, and I is the discharge current; preferably, the standing time is 8-48 h.
6. The method of any of claims 1-5, wherein the pre-lithiation process comprises pre-lithiation of lithium in a mass M ═ M × C × a × 3600)/F, where M is the molar mass of lithium, F is the faraday constant, C is the capacity of the negative electrode, and a is the percentage of the pre-lithiation capacity to the negative electrode capacity.
7. The electrochemical uniform pre-lithiation method for lithium ion batteries according to any one of claims 1 to 6, characterized in that the total thickness of the metallic lithium layers on both sides is > m/(ρ A), ρ is the density of the metallic lithium and A is the surface area of the metallic lithium layer.
8. The electrochemical uniform pre-lithium method for the lithium ion battery according to any one of claims 1 to 7, wherein the thickness of the copper foil in the copper-lithium composite layer is 4 to 15 μm.
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