CN114361436A - Square cylindrical lithium cobalt oxide battery and preparation method thereof - Google Patents

Square cylindrical lithium cobalt oxide battery and preparation method thereof Download PDF

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CN114361436A
CN114361436A CN202111677891.0A CN202111677891A CN114361436A CN 114361436 A CN114361436 A CN 114361436A CN 202111677891 A CN202111677891 A CN 202111677891A CN 114361436 A CN114361436 A CN 114361436A
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slurry
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CN114361436B (en
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高峰
雷飞叶
张要枫
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Hubei Titanium Era New Energy Co Ltd
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
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Abstract

The invention provides a square cylindrical lithium cobalt oxide battery and a preparation method thereof, wherein the battery is of a square cylindrical structure, a shell is a cube, a cylindrical battery cell is arranged in the shell, and a bracket is arranged between two ends of the cylindrical battery cell and the inner wall of the shell; the cylindrical battery cell comprises a central tube, and is formed by winding a composite film formed by laminating a positive plate, a diaphragm and a negative plate along the central tube; electrolyte is also injected into the shell; the positive active material of the positive plate is lithium cobaltate, and the negative active material of the negative plate is lithium titanate. During specific preparation, respectively preparing anode slurry and cathode slurry, and respectively coating the anode slurry and the cathode slurry on an aluminum foil to prepare an anode plate and a cathode plate; and assembling the positive plate, the diaphragm and the negative plate by a winding process, putting the positive plate, the diaphragm and the negative plate into a shell, injecting electrolyte into the shell, and finally forming the battery through aging and capacity grading. The battery provided by the invention is simple to assemble, and can improve the safety of the battery and prolong the cycle life of the battery.

Description

Square cylindrical lithium cobalt oxide battery and preparation method thereof
Technical Field
The invention belongs to the field of battery materials, and particularly relates to a square cylindrical lithium cobalt oxide battery and a preparation method thereof.
Background
With the rapid development of the lithium battery industry, the high rate, high energy density, long cycle, high voltage and high safety performance of lithium cobalt oxide batteries have become the key content in the research of lithium cobalt oxide materials; however, the problems of explosion and fire, low energy density, short cycle life and the like frequently occur in the use of the lithium battery; the traditional lithium cobaltate battery adopts a soft package, a pure square or a pure cylindrical structure; the pure square battery structure is easy to bulge and deform due to excessive internal gas, and explosion is caused when the internal gas is serious; the pure cylindrical battery has small internal space and cannot bear more gas, so the battery needs to be frequently exhausted. Although the soft packaging process can improve the energy density of the battery, the consistency of the thickness of the pole piece is poor, so that the pole piece has large errors in assembly and overall size.
Disclosure of Invention
The invention provides a square cylindrical lithium cobaltate battery and a preparation method thereof, wherein a square cylindrical structure is adopted, the square cylindrical structure has the advantages of being square and cylindrical, the preparation method is simple, the safety of the battery can be improved, the cycle life of the battery can be prolonged, and the problem of thickness consistency is solved.
The technical scheme of the invention is that the square cylindrical lithium cobalt oxide battery is of a square cylindrical structure, wherein a shell is a cube, a cylindrical battery cell is arranged in the shell, and a bracket is arranged between two ends of the cylindrical battery cell and the inner wall of the shell; the cylindrical battery cell comprises a central tube, and is formed by winding a composite film formed by laminating a positive plate, a diaphragm and a negative plate along the central tube; electrolyte is also injected into the shell; the positive active material of the positive plate is lithium cobaltate, and the negative active material of the negative plate is lithium titanate.
Further, casing one end is equipped with anodal subassembly, and the other end is equipped with the negative pole subassembly, and anodal subassembly and negative pole subassembly are connected respectively to the both ends of center tube.
Furthermore, supporting legs are arranged around the support, the support is connected to the inner wall of the shell in a clamping mode through the supporting legs, the supporting legs are of an inner hollow structure, and two ends of the supporting legs are open.
Further, the positive plate comprises a positive current collector and positive slurry coated on the positive current collector, wherein the positive slurry comprises positive active material lithium cobaltate, a binder, a conductive agent and a solvent; the negative plate comprises a negative current collector and negative slurry coated on the negative current collector, wherein the negative slurry comprises negative and positive active lithium titanate, a binder, a conductive agent and a solvent.
In the preferred positive electrode slurry, 85-91% by weight of lithium cobaltate, 2-5% by weight of a binder, 4-8% by weight of a conductive agent and 3-6% by weight of an NMP solvent are added, and the sum of the components is 100%.
In the preferable negative electrode slurry, 82-92% of lithium titanate, 2-7% of a negative electrode binder, 3-8% of a negative electrode conductive agent and 3-7% of an NMP solvent are calculated according to weight percentage, and the sum of the components is 100%.
Further, the conductive agent is one or more of conductive carbon black, carbon nanotubes, conductive graphite and carbon fibers. Conductive agents consisting of conductive carbon black and carbon nanotubes are preferred. The binder is polyvinylidene fluoride, and the solvent is N-methyl pyrrolidone.
Further, the thickness of the aluminum foil is 8-12 μm, and the coating thickness of the anode slurry and the cathode slurry is 80-90 μm respectively.
Further, the electrolyte is lithium hexafluorophosphate. Wherein the content of lithium ions is 6-7 times of that of common electrolyte, and the conductivity is strong.
The invention also relates to a method for preparing the square cylindrical lithium cobalt oxide battery, which comprises the following specific steps:
s1, preparing positive electrode slurry: preparing a binding agent into binding solution by using a solvent, dissolving the carbon nano tube and the binding agent into the solvent to prepare conductive slurry, uniformly mixing the conductive slurry and conductive carbon black, adding dried lithium cobaltate, and adjusting solid content to prepare anode slurry;
s2, preparing anode slurry: preparing a binding agent into binding solution by using a solvent, and then dissolving the carbon nano tube and the binding agent into the solvent to prepare conductive slurry; mixing the conductive slurry with conductive carbon black, finally adding dried lithium titanate, and adjusting solid content to prepare cathode slurry;
s3, respectively coating the positive electrode slurry and the negative electrode slurry on an aluminum foil, and then rolling, slitting and baking to prepare a positive plate and a negative plate;
and S4, assembling the positive plate, the diaphragm and the negative plate by a winding process, putting the positive plate, the diaphragm and the negative plate into a square cylindrical shell, injecting electrolyte into the square cylindrical shell, and finally forming the battery through aging and capacity grading.
Further, the lithium cobaltate material and the lithium titanate material are dried for 12-15h at the temperature of 100 ℃ and 120 ℃ before being used.
Further, the solid content of the positive electrode slurry in the S1 is 50-65%; the solid content of the negative electrode slurry in S2 is 50-65%.
The invention has the following beneficial effects:
1. lithium cobaltate is used as a positive electrode material, lithium titanate is used as a negative electrode material, and lithium titanate is a zero-strain material, so that lithium ions cannot generate dendrites in the de-intercalation process, and the safety of the battery is improved;
2. the battery adopts a square cylindrical structure, and the corresponding positioning mechanisms are arranged among all the parts, so that the matching precision among all the parts can be obviously improved, the assembly of an installer is convenient, the assembly efficiency of the installer is improved, and the assembly precision of the lithium battery is also improved;
3. the square battery shell is adopted during the assembly of the battery, the electrolyte bearing capacity in the battery can be obviously improved under the same volume, and the cycle life of the battery is prolonged.
Drawings
Fig. 1 is an exploded view of the overall appearance structure of a prismatic battery.
Fig. 2 is an exploded view of the cathode assembly structure of a prismatic cylindrical battery.
Fig. 3 is a sectional view of the structure of the prismatic battery in an assembled state.
Fig. 4 is an appearance view of the prismatic battery in an assembled state.
Fig. 5 is a schematic structural view of a square cylindrical battery exhaust device.
Fig. 6 is a charge and discharge curve of a prismatic battery of example 3.
Fig. 7 is a graph of the cycle number of prismatic cells of example 3.
In the figure: the battery comprises a negative electrode assembly 1, a sealing screw 101, a negative electrode cover plate 102, a negative electrode support 103, a negative electrode post 104, a negative electrode plate 105, a mounting notch 1051, a sealing washer 106, an exhaust hole 107, a central tube 2, a battery shell 3, a connecting plunger 4, a positive electrode assembly 5, a first insulating sealing ring 501, a positive electrode cover plate 502, a second insulating sealing ring 503, a positive electrode support 504, a positive electrode post 505 and a positive electrode plate 506.
Detailed Description
Embodiments of the present invention will be described in detail below with reference to examples, but those skilled in the art will appreciate that the following examples are only illustrative of the present invention and should not be construed as limiting the scope of the present invention.
The structure of the square cylindrical battery is shown in fig. 1-5, and comprises a battery shell 3, a cylindrical battery core is arranged in the battery shell, and supports 103 and 504 are arranged between two ends of the cylindrical battery core and the inner wall of the shell; the cylindrical battery cell comprises a central tube, and is formed by winding a composite film formed by laminating a positive plate, a diaphragm and a negative plate along the central tube; electrolyte is also injected into the shell.
In the preferred scheme, casing one end is equipped with anodal subassembly, and the other end is equipped with the negative pole subassembly, and anodal subassembly and negative pole subassembly are connected respectively to the both ends of center tube. The both ends of preferred center tube 2 are through connecting plunger 4 and negative pole subassembly 1 and the 5 joint of positive pole subassembly, center tube 2 is connected into a whole with negative pole subassembly 1 and positive pole subassembly 5 in battery case 3's inside, center tube 2's axle center and positive pole subassembly 5, three coincidence between the negative pole subassembly 1, center tube 2 owing to with be provided with clamping mechanism between positive pole subassembly 5 and the negative pole subassembly 1, center tube 2 can not take place to rock and drop when the battery is in operation, and then promoted the stability of battery operation by a wide margin.
In the preferred scheme, positive subassembly 5 includes anodal apron 502, anodal support 504, anodal utmost point post 505 and anodal polar plate 506, anodal support 504 is installed in battery case 3, and anodal apron 502 is connected to the up end of anodal support 504, and anodal polar plate 506 is connected to the lower terminal surface of positive subassembly 5, and anodal utmost point post 505 run through and connect anodal apron 502 and anodal support 504 and install in negative pole polar plate 105, and anodal apron 502 is welded fastening with battery case 3 outside the battery, can guarantee the stability after the installation of anodal utmost point post 505 through this structure, prevents to take place to rock and drop in the in-process of operation, has also guaranteed the leakproofness between anodal subassembly 5 and the battery case 3.
In a further preferable scheme, a first insulating sealing ring 501 is arranged on the contact surface of the positive pole post 505 outside the battery and the positive cover plate 502, a second insulating sealing ring 503 is arranged on the contact surface of the positive pole post 505 inside the battery and the positive cover plate 502, the sealing performance of the positive pole post 505 outside the battery can be ensured through the first insulating sealing ring 501, the sealing performance of the positive pole post 505 inside the battery can be ensured through the second insulating sealing ring 5013, and further the absolute sealing of the positive pole assembly is ensured, so that the electrolyte in the battery shell 3 is prevented from leaking out, and meanwhile, the insulating performance of components around the positive pole post 505 is also ensured.
In a preferred scheme, the negative electrode assembly 1 comprises a sealing screw 101, a negative electrode cover plate 102, a negative electrode support 103, a negative electrode post 104 and a negative electrode plate 105, the negative electrode support 103 is arranged in the battery shell 3, the lower end face of the negative electrode support 103 is connected with the negative electrode plate 105, the upper end face of the negative electrode support 103 is connected with the negative electrode cover plate 102, an installation notch 1051 is formed in the axis of the negative electrode plate 105, the negative electrode post 104 penetrates through the negative electrode support 103 and the negative electrode cover plate 102 and is clamped in the installation notch 1051, the negative electrode cover plate 102 is welded and fixed with the battery shell 3 outside the battery, the stability of the negative electrode post 104 after installation can be ensured through the structure, and the negative electrode post 104 is prevented from shaking and falling off due to external reasons during operation.
In a further preferred scheme, the sealing screw 101 is in threaded connection with the negative pole 104, a sealing washer 106 is arranged on the inner contact surface of the sealing screw 101 and the negative pole 104, an exhaust hole 107 is formed in the side wall of the negative pole 104, and the exhaust hole 107 is communicated with the inside of the negative pole 104; when the sealing screw 101 is rotated upwards, the lower end of the sealing screw 101 is connected with the sealing washer 106 and moves upwards synchronously, the sealing washer 106 can leave from the exhaust hole 107, the inside of the sealing screw 101 is communicated with the outside, gas in the battery can be exhausted through the exhaust hole 107, and meanwhile, electrolyte can be filled into the battery through the exhaust hole 107; when the sealing screw 101 is rotated downwards, the lower end of the sealing screw 101 is connected with the sealing washer 106 and synchronously moves downwards, the sealing washer 106 moves downwards and blocks the exhaust hole 107, and the inside of the sealing screw 101 is sealed.
Supporting legs are arranged on the periphery of the support, the support is connected to the inner wall of the shell in a clamping mode through the supporting legs, the supporting legs are of an inner hollow structure, and two ends of the supporting legs are open. The hollow supporting leg structure can improve the internal space of the battery shell, so that the internal part of the battery shell can provide a larger storage space for electrolyte, the cycle service life of the battery is prolonged, and meanwhile, a buffer storage space is provided for gas generated in the battery shell in the using process of the battery.
Example 1
A square cylindrical lithium cobalt oxide battery,
a positive electrode material: 91% of lithium cobaltate, 2% of polyvinylidene fluoride, 4% of conductive agent consisting of 2% of conductive carbon black and 2% of carbon nano tube, and 3% of solvent N-methyl pyrrolidone;
the specific surface area of the positive plate is 0.230m2(ii)/g, tap density 0.76g/cm3The water content was 300 ppm.
And (3) anode material: 92% of lithium titanate, a negative electrode binder PVDF 2%, 3% of a negative electrode conductive agent (wherein the conductive carbon black accounts for 1.3% and the carbon nano tube accounts for 1.7%), and 3% of a solvent N-methylpyrrolidone.
The specific surface area of the negative pole piece is 1.98m2(ii)/g, tap density 0.68g/cm3The water content was 200 ppm.
The specific preparation method of the battery comprises the following steps:
preparing anode slurry:
step a): drying the lithium cobaltate positive electrode material at the temperature of 100-120 ℃ for 12 h;
step b): dissolving a binder in an N-methyl pyrrolidone (chemical formula is abbreviated as NMP) solvent to prepare a binder solution, and then dissolving carbon nanotubes in the NMP solvent to prepare conductive slurry;
step c): dissolving the conductive slurry and the dried conductive carbon black in the binding liquid, stirring for 2 hours, adding the dried lithium cobaltate anode material, supplementing a proper amount of NMP solvent, and continuously stirring for 3 hours to prepare anode slurry;
preparing anode slurry:
step a): dissolving a binder in an N-methyl pyrrolidone (chemical formula is abbreviated as NMP) solvent to prepare a binder solution, and then dissolving the carbon nano tube and a dispersing agent in the NMP solvent to prepare a conductive slurry;
step b): dissolving the conductive slurry and the dried conductive carbon black in the binding liquid, stirring for 2 hours, adding the dried lithium titanate negative electrode material, supplementing a proper amount of NMP solvent to adjust the solid content to 65%, and continuously stirring for 4 hours to prepare negative electrode slurry;
preparing a pole piece: coating the positive electrode slurry on an aluminum foil with the thickness of 8 mu m, coating the negative electrode slurry carbon material on the aluminum foil with the thickness of 8 mu m, rolling (the coating speed is 9 m/min; the oven temperature is 120 +/-5 ℃, the ambient temperature is 25 +/-5 ℃, the ambient relative humidity is less than 25 percent RH), the rolling speed is 20 m/min; the pressure is 6MPa), cutting, baking (the baking time is 28h, the temperature is 120 +/-2 ℃) and obtaining a positive plate and a negative plate;
preparing an electric core: and assembling the positive plate, the diaphragm and the negative plate along the central tube by a winding process, putting the assembled positive plate, the diaphragm and the negative plate into a battery shell, injecting lithium hexafluorophosphate electrolyte into the battery shell, and finally forming the battery through aging and grading.
Example 2: the positive electrode was identical to example 1, and the negative electrode material: 85% of lithium titanate, a negative binder PVDF 5%, 6% of a negative conductive agent (wherein the conductive carbon black accounts for 2% and the carbon nano tube accounts for 4%), and 4% of a solvent N-methylpyrrolidone.
Example 3: the positive electrode was identical to example 1, and the negative electrode material: 90% of lithium titanate, 2% of negative electrode binder PVDF, 4% of negative electrode conductive agent (wherein the conductive carbon black accounts for 2% and the carbon nano tube accounts for 2%), and 4% of solvent N-methyl pyrrolidone.
Comparative example 1: the positive and negative electrodes were made into pouch cells in the same manner as in example 1.
Comparative example 2: the positive and negative electrodes were identical to those of example 1, but they were fabricated into cylindrical batteries.
Comparative example 2: the positive and negative electrodes were identical to those of example 1, but they were fabricated into prismatic cells.
The batteries prepared in the above examples and comparative examples were subjected to performance tests, and the performances thereof were compared as shown in table 1 below.
TABLE 1
Figure BDA0003452795690000051
Figure BDA0003452795690000061
Fig. 6 is a charge-discharge curve of the prismatic battery of example 3, which can realize fast charge to 90% of electric quantity in 6 min. FIG. 7 is a graph of the cycle number of prismatic cells of example 3, which shows almost no change in performance after 20000 cycles.
The square cylindrical battery prepared by the method provided by the invention has better performances than the traditional soft package, cylindrical battery and square battery.

Claims (10)

1. The utility model provides a square cylinder lithium cobalt oxide cell which characterized in that: the battery is of a square cylindrical structure, wherein the shell is a cube, a cylindrical battery cell is arranged in the shell, and a bracket is arranged between two ends of the cylindrical battery cell and the inner wall of the shell; the cylindrical battery cell comprises a central tube, and is formed by winding a composite film formed by laminating a positive plate, a diaphragm and a negative plate along the central tube; electrolyte is also injected into the shell; the positive active material of the positive plate is lithium cobaltate, and the negative active material of the negative plate is lithium titanate.
2. The battery of claim 1, wherein: casing one end is equipped with anodal subassembly, and the other end is equipped with the negative pole subassembly, and anodal subassembly and negative pole subassembly are connected respectively to the both ends of center tube.
3. The battery of claim 1, wherein: supporting legs are arranged on the periphery of the support, the support is connected to the inner wall of the shell in a clamping mode through the supporting legs, the supporting legs are of an inner hollow structure, and two ends of the supporting legs are open.
4. The battery of claim 1, wherein the positive electrode sheet comprises a positive current collector and a positive electrode slurry coated thereon, the positive electrode slurry comprising a positive active material lithium cobaltate, a binder, a conductive agent, and a solvent; the negative plate comprises a negative current collector and negative slurry coated on the negative current collector, wherein the negative slurry comprises negative active material lithium titanate, a binder, a conductive agent and a solvent.
5. The battery according to claim 3 or 4, wherein: the conductive agent is one or more of conductive carbon black, carbon nano tubes, conductive graphite and carbon fibers, the binder is polyvinylidene fluoride, and the solvent is N-methylpyrrolidone.
6. The square cylindrical lithium cobaltate battery as defined in claim 4, wherein: the thickness of the positive current collector and the negative current collector is 8-12 mu m, and the coating thickness of the positive electrode slurry and the coating thickness of the negative electrode slurry are 80-90 mu m respectively.
7. The square cylindrical lithium cobaltate battery as defined in claim 1, wherein: the electrolyte is lithium hexafluorophosphate.
8. The method for preparing the square cylindrical lithium cobalt oxide battery as claimed in any one of claims 1 to 7, which comprises the following specific steps:
s1, preparing positive electrode slurry: preparing a binding agent into binding solution by using a solvent, dissolving the carbon nano tube and the binding agent into the solvent to prepare conductive slurry, uniformly mixing the conductive slurry and conductive carbon black, adding dried lithium cobaltate, and adjusting solid content to prepare anode slurry;
s2, preparing anode slurry: preparing a binding agent into binding solution by using a solvent, and then dissolving the carbon nano tube and the binding agent into the solvent to prepare conductive slurry; mixing the conductive slurry with conductive carbon black, finally adding dried lithium titanate, and adjusting solid content to prepare cathode slurry;
s3, respectively coating the positive electrode slurry and the negative electrode slurry on an aluminum foil, and then rolling, slitting and baking to prepare a positive plate and a negative plate;
and S4, assembling the positive plate, the diaphragm and the negative plate by a winding process, putting the positive plate, the diaphragm and the negative plate into a square cylindrical shell, injecting electrolyte into the square cylindrical shell, and finally forming the battery through aging and capacity grading.
9. The method of claim 8, wherein: the lithium cobaltate material and the lithium titanate material are dried for 12-15h at the temperature of 100-120 ℃ before use.
10. The method of claim 8, wherein: the solid content of the positive electrode slurry in S1 is 50-65%; the solid content of the negative electrode slurry in S2 is 50-65%.
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CN202217738U (en) * 2011-08-31 2012-05-09 浙江谷神能源科技股份有限公司 Low-voltage anti-explosion cylindrical lithium ion battery
CN109786589A (en) * 2019-01-04 2019-05-21 上海德朗能动力电池有限公司 A kind of battery modules of square lithium ion battery and preparation method and its composition
CN110176623A (en) * 2019-06-10 2019-08-27 合肥众禾动力新能源科技有限公司 A kind of preparation method of lithium ion battery
CN214706018U (en) * 2021-03-03 2021-11-12 银隆新能源股份有限公司 Lithium ion power battery
CN214848830U (en) * 2021-04-19 2021-11-23 武汉蔚能电池资产有限公司 Battery pack packaging structure

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2002208380A (en) * 2001-01-09 2002-07-26 Matsushita Electric Ind Co Ltd Battery and its manufacturing method
CN202167563U (en) * 2011-07-26 2012-03-14 珠海银通新能源有限公司 Cylindrical lithium-ion power battery
CN202217738U (en) * 2011-08-31 2012-05-09 浙江谷神能源科技股份有限公司 Low-voltage anti-explosion cylindrical lithium ion battery
CN109786589A (en) * 2019-01-04 2019-05-21 上海德朗能动力电池有限公司 A kind of battery modules of square lithium ion battery and preparation method and its composition
CN110176623A (en) * 2019-06-10 2019-08-27 合肥众禾动力新能源科技有限公司 A kind of preparation method of lithium ion battery
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