WO2022068207A1 - 一种复合集流体、制备方法及锂离子电池 - Google Patents

一种复合集流体、制备方法及锂离子电池 Download PDF

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Publication number
WO2022068207A1
WO2022068207A1 PCT/CN2021/092598 CN2021092598W WO2022068207A1 WO 2022068207 A1 WO2022068207 A1 WO 2022068207A1 CN 2021092598 W CN2021092598 W CN 2021092598W WO 2022068207 A1 WO2022068207 A1 WO 2022068207A1
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Prior art keywords
conductor layer
current collector
composite current
area
layer
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PCT/CN2021/092598
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English (en)
French (fr)
Inventor
张磊
王晓明
魏凤杰
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江苏卓高新材料科技有限公司
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Priority to EP21873870.6A priority Critical patent/EP4224581A1/en
Priority to US18/247,204 priority patent/US20230378477A1/en
Publication of WO2022068207A1 publication Critical patent/WO2022068207A1/zh

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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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • 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
    • H01M10/04—Construction or manufacture in general
    • 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
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H01M4/662—Alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/668—Composites of electroconductive material and synthetic resins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/043—Processes of manufacture in general involving compressing or compaction
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • 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
    • 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
    • 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
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present application relates to the technical field of secondary batteries, for example, to a composite current collector, a preparation method and a lithium ion battery.
  • Lithium-ion batteries are formed by winding or superimposing a basic unit structure, and the basic unit structure is positive electrode/separator/negative electrode.
  • the positive electrode and the negative electrode are the places where the electrochemical reaction occurs.
  • the current generated by the electrochemical reaction is collected and exported through the current collectors in the positive electrode and the negative electrode. .
  • the common configuration of the current collector is to use copper foil material for the negative electrode and aluminum foil material for the positive electrode. Due to the use of metal materials, the positive and negative current collectors occupy a large proportion (about 8%) in the total weight of the cell, so reducing the weight of the current collector is an effective way to improve the energy density (kWh/kg) of lithium-ion batteries.
  • Chinese patent applications CN106654285A and CN101071860A can prepare low-density current collectors by preparing conductive plating layers on the surface of flexible substrates.
  • Another example is the Chinese patent application with the publication number CN110277532A, which discloses a processing method and processing equipment for a secondary battery current collector. The current in the cell is delivered.
  • CN110165223A discloses a composite current collector with a porous structure and a conductor layer inside the hole, which can realize conduction between the metal conductor layers on both sides of the composite current collector.
  • a current collector needs to be punched, and the conductor layer inside the hole is difficult to manufacture, and the conduction effect is poor, which is not conducive to the popularization and application of the composite current collector.
  • the utility model with the authorization announcement number CN208051145U discloses an ultrasonic welding head and welding equipment. Through the extrusion of the conical structure of the welding head during welding, the polymer layer in the welding area is penetrated, and the metal conductor layers in the welding area are welded together, and the two metal conductor layers are connected to each other during welding. However, this welding process can easily lead to over-soldering, destroying the metal conductor layer in the welding area, low welding strength and poor electrical conductivity.
  • the present application provides a composite current collector, which improves the situation that the tab welding of the composite current collector is difficult in the related art, and simultaneously improves the situation that the conductor layers on both sides of the composite current collector are difficult to conduct.
  • a composite current collector comprising: a support layer, the support layer is made of a polymer; a first conductor layer, the first conductor layer is disposed on one side of the support layer; A second conductor layer, the second conductor layer is disposed on the other side of the support layer; a welding area; wherein, in the welding area, there is no polymer between the first conductor layer and the second conductor layer.
  • the embodiment of the present application also discloses a preparation method of a composite current collector, which is used to prepare the composite current collector as described above.
  • the current collector includes a conductor layer and a support layer, and includes the following steps: compressing the conductor layer material into a the conductor layer, and composite the conductor layer on the first side and the second side of the support layer.
  • the embodiment of the present application further discloses a lithium ion battery, comprising a positive electrode piece, a negative electrode piece, a separator and an electrolyte, wherein the positive electrode piece and/or the negative electrode piece include the composite current collector as described above.
  • FIG. 1 is a schematic structural diagram of a composite current collector in an embodiment of the present application.
  • FIG. 2 is a plan view of the composite current collector shown in FIG. 1 .
  • FIG. 3A is a schematic structural diagram of a composite current collector in another embodiment of the present application.
  • Figure 3 is a top view of the composite current collector shown in Figure 3A.
  • FIG. 4 is a schematic structural diagram of a composite current collector in a third embodiment of the present application.
  • FIG. 5 is a schematic structural diagram of a composite current collector in a fourth embodiment of the present application.
  • FIG. 6 is a schematic structural diagram of a composite current collector in a fifth embodiment of the present application.
  • Support layer 2. First conductor layer 3. Second conductor layer
  • the terms “installed”, “connected” and “connected” should be understood in a broad sense, for example, it may be a fixed connection or a detachable connection Connection, or integral connection; can be mechanical connection, can also be electrical connection; can be directly connected, can also be indirectly connected through an intermediate medium, can be internal communication between two elements.
  • installed should be understood in a broad sense, for example, it may be a fixed connection or a detachable connection Connection, or integral connection; can be mechanical connection, can also be electrical connection; can be directly connected, can also be indirectly connected through an intermediate medium, can be internal communication between two elements.
  • the present application shows a schematic structural diagram of a composite current collector through FIG. 1
  • FIG. 2 is a top view of the composite current collector shown in FIG. 1
  • the composite current collector includes a support layer 1, a first conductor layer 2 and a second conductor layer 3, and the first conductor layer 2 and the second conductor layer 3 are respectively compounded on the support layer 1 on both sides.
  • the support layer 1 is made of a polymer material for providing support force.
  • the first conductor layer 2 and the second conductor layer 3 generally use the same conductive material for conducting current.
  • the dotted line indicates the intersection position of the first conductor layer 2 and the second conductor layer 3 and the support layer 1
  • the hatched line indicates the bonding area 4 .
  • the above-mentioned composite current collector further includes at least one welding area 4, in which there is no welding area between the first conductor layer 2 and the second conductor layer 3.
  • the polymer used to prepare the support layer 1 (thus the weld area 4 in Figure 2 does not extend to the dotted line).
  • the welding area 4 without polymer is provided.
  • the mutual electrical connection between the first conductor layer 2 and the second conductor layer 3 can be realized without penetrating the support layer 1, and then the first conductor layer 2 and the current generated on the second conductor layer 3 are derived, which improves the situation that the tab welding of the composite current collector is difficult in the related art and the situation that the conductor layers on both sides of the composite current collector are difficult to achieve conduction.
  • the polymer material used in the support layer 1 is polyethylene terephthalate (Polyethylene terephthalate, PET), polypropylene (Polypropylene, PP), polyethylene (Polyethylene, PE), polyimide (Polyimide) , PI), one or more of polyarylsulfone, or other insulating materials with light weight and high strength can be used as an alternative.
  • the thickness of the support layer 1 is 2 micrometers to 6 micrometers.
  • the first conductor layer 2 and the second conductor layer 3 can be made of aluminum, copper, nickel, silver, gold, carbon, stainless steel or alloys thereof.
  • the first conductor layer 2 and the second conductor layer 3 used as the positive electrode current collector are generally made of aluminum or aluminum alloy materials
  • the first conductor layer 2 and the second conductor layer 3 used as the negative electrode current collector are generally made of aluminum or aluminum alloy materials.
  • the thickness of the first conductor layer 2 and the second conductor layer 3 is 0.2-5 microns. If the thickness of the first conductor layer 2 and the second conductor layer 3 is less than 0.2 microns, the electrical conductivity is insufficient and the internal resistance is large; if the thickness exceeds 5 microns, the thickness and weight are too large, which affects the energy density of the battery.
  • the area of the soldering region 4 accounts for 0.5-30% of the area of the first conductor layer 2 (or the second conductor layer 3 ). If the area ratio of the welding area 4 exceeds 30%, the first conductive layer 2 and the second conductive layer 3 do not have enough supporting area (provided by the supporting body layer 1 ) and are easily damaged. If the area ratio of the welding area is less than 0.5%, a sufficient area cannot be provided for welding the tabs.
  • the welding area 4 may be implemented in various shapes such as rectangle, circle, ellipse, fan shape, polygon or irregular shape, which does not limit the present application.
  • the welding area 4 can also be set at any position on the composite current collector, and in one embodiment, can be set on the edge of the composite current collector, which facilitates subsequent welding of the tabs.
  • the direction represented by W is the width direction
  • the welding area 4 is formed by the width of the first conductor layer 2 and the second conductor layer 3 being wider than that of the support layer 4, so that the When the first conductor layer 2 and the second conductor layer 3 are composited on both sides of the support layer 4 , a welding area 4 is naturally formed at the edge of the composite current collector, and no additional operations on the support layer 4 are required.
  • FIG. 3A shows a schematic structural diagram of a composite current collector in another embodiment of the present application
  • FIG. 3 is a top view of the composite current collector shown in FIG. 3A
  • the welding area 4 can also be formed by hollowing out the support layer.
  • the hollow area is represented by the hatched line in Figure 3. There is no hollow area at A-A' in the figure, and a hollow area (that is, welding area 4) is set at B-B'.
  • FIG. 4 shows the structure of the composite current collector in the third embodiment of the present application.
  • FIG. 4 is based on FIG. 1 , the thickness of the first conductor layer 2 and/or the second conductor layer 3 in the welding area 4 is made larger than the remaining part thereof to form a thickened area.
  • the thickness of the thickened region in the welding region 4 is h2 , and the thickness of the remaining portion is h1 , and h2 > h1 .
  • the strength of the welding area 4 can be enhanced to avoid damage during processing; the thickness of the first conductor layer 2 and the second conductor layer 3 to be welded can also be enhanced to improve the welding strength.
  • FIG. 5 shows the structure of the composite current collector in the fourth embodiment of the present application.
  • Figure 5 is based on Figure 4, the direction represented by W is the width direction, the edge of the thickened area is wider than the welding area 4, and the width is 0.5-10mm, so that the edge of the thickened area overlaps with the edge of the support layer 1, enhancing the The strength of the welding area 4 prevents the conductor layer from breaking at the edge of the welding area 4 .
  • FIG. 6 shows the structure of the composite current collector in the fifth embodiment of the present application.
  • a conductive adhesive 5 is filled between the first conductor layer 2 and the second conductor layer 3 in the welding area 4.
  • the bonding of the conductive adhesive 5 can improve the strength of the welding area 4 and avoid the If damaged, the strength of the first conductor layer 2 and the second conductor layer 3 after soldering can also be improved.
  • the preparation method of the composite current collector may include the following steps: after the conductor layer material is pressed into the conductor layer, the conductor layer and the support layer material are compounded. Wherein, the conductor layer and the support layer can be connected and combined by an adhesive. The completed composite conductor layer can be thinned by chemical or electrochemical methods.
  • the cover can be tape, which needs to be removed after thinning is complete.
  • the above-mentioned composite current collector can be used to make a pole piece: the positive electrode active material is coated on the surface of the current collector to obtain a positive electrode pole piece; the negative electrode active material is coated on the surface of the current collector to prepare a negative electrode pole piece.
  • the positive pole piece, the separator and the negative pole piece are assembled in a winding manner to form a dry cell.
  • the dry cell is put into the battery case and the electrolyte is injected, and the secondary battery is prepared by charging and forming.
  • the aluminum material with a purity of 99.7% is rolled to obtain an aluminum foil with a thickness of 5 microns.
  • a 5-micron-thick aluminum foil is laminated on both sides of a 5-micron-thick PET through an adhesive to form a positive current collector.
  • the molecular weight of PET is 192.17
  • the adhesive is WB888 produced by Wuxi Yuke
  • the compounding temperature is 95 degrees Celsius
  • the compounding pressure is 0.5 MPa
  • the standing time after compounding is 150 hours.
  • the width of 5 micron aluminum foil is 100mm
  • the width of PET is 80mm.
  • the area ratio of the welding area is 20%.
  • the thickness of the above-mentioned single-sided aluminum layer after chemical etching is 3 microns.
  • Example 2 The difference between Example 2 and Example 1 is that a 4-micron-thick PET material is used as the support layer, and a 3-micron-thick aluminum foil is used as the conductor layer; the width of the aluminum foil is 100 mm, the width of the PET is 90 mm, and the area ratio of the welding area is 10%. %.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area, and the width of the thickened area is 1 mm wider than the welding area.
  • the thickness of the thickened area is 3 microns, and the thickness of the remaining areas is 2 microns.
  • Example 3 The difference between Example 3 and Example 1 is that PP material with a thickness of 3 microns is used as the support layer, and aluminum foil with a thickness of 5 microns is used as the conductor layer; the width of the aluminum foil is 100 mm, the width of PET is 95 mm, and the area ratio of the welding area is 5 %.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area.
  • the thickness of the thickened area is 5 microns, and the thickness of the remaining areas is 2 microns.
  • Example 4 The difference between Example 4 and Example 1 is that PE material with a thickness of 2 microns is used as the support layer, and aluminum foil with a thickness of 10 microns is used as the conductor layer; the width of the aluminum foil is 100 mm, the width of PET is 70 mm, and the area ratio of the welding area is 30 mm. %.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area.
  • the thickness of the thickened area is 10 microns, and the thickness of the remaining area is 5 microns. Also, fill the soldered area with conductive glue.
  • Example 5 The difference between Example 5 and Example 1 is that PI material with a thickness of 6 microns is used as the support layer, and aluminum foil with a thickness of 2 microns is used as the conductor layer; the width of the aluminum foil is 100 mm, the width of the PET is 75 mm, and the area ratio of the welding area is 25 mm. %.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area.
  • the thickness of the thickened area is 2 microns, and the thickness of the remaining areas is 0.5 microns. Also, fill the soldered area with conductive glue.
  • the copper with a purity of 99.7% was rolled to obtain a copper foil with a thickness of 5 microns.
  • a 5-micron-thick copper foil is laminated on both sides of a 5-micron-thick PET through an adhesive to form a positive current collector.
  • the molecular weight of PET is 192.17
  • the adhesive is WB888 produced by Wuxi Yuke
  • the compounding temperature is 95 degrees Celsius
  • the compounding pressure is 0.5 MPa
  • the standing time after compounding is 150 hours.
  • the width of the 4-micron copper foil is 100mm
  • the width of the PET is 80mm
  • the area ratio of the welding area is 20%.
  • the temperature is 45 degrees Celsius, the corrosion time is 1 minute, and then use deionized water to rinse and dry.
  • the thickness of the above-mentioned single-sided copper foil is 4 microns after chemical etching.
  • Example 7 The difference between Example 7 and Example 6 is that PP material with a thickness of 4 microns is used as the support layer, and copper foil with a thickness of 6 microns is used as the conductor layer; the width of the copper foil is 100 mm, the width of the PET is 90 mm, and the The area ratio is 10%; the thickness of the thinned single-sided copper foil is 5 microns.
  • Example 8 The difference between Example 8 and Example 6 is that a 3-micron-thick PET material is used as the support layer, and a 3-micron-thick copper foil is used as the conductor layer; the width of the copper foil is 100 mm, the width of the PET is 99 mm, and 1% of the area
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area, and the width of the thickened area is 0.5 mm wider than the welding area.
  • the thickness of the thickened area is 3 microns, and the thickness of the remaining areas is 1 micron.
  • Example 9 The difference between Example 9 and Example 6 is that a 2-micron-thick polyarylsulfone material is used as the support layer, and a 3-micron-thick copper foil is used as the conductor layer; the width of the copper foil is 100mm, the width of the PET is 85mm, and The area ratio is 15%.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area.
  • the thickness of the thickened area is 3 microns, and the thickness of the remaining areas is 0.5 microns. Also, fill the soldered area with conductive glue.
  • Example 10 The difference between Example 10 and Example 6 is that PE material with a thickness of 5 microns is used as the support layer, and copper foil with a thickness of 6 microns is used as the conductor layer; the width of the copper foil is 100 mm, the width of PET is 70 mm, and the area of the welding area is ratio of 30%.
  • the surface of the conductor layer on the welding area is covered with tape to form a thickened area.
  • the thickness of the thickened area is 6 microns, and the thickness of the remaining areas is 2 microns. Also, fill the soldered area with conductive glue.
  • Comparative Example 1 The difference between Comparative Example 1 and Example 1 is that the width of the aluminum foil is the same as that of the PET, and there is no welding area.
  • Comparative Example 2 The difference between Comparative Example 2 and Example 1 is that a PP material with a thickness of 4 ⁇ m is used as the support layer, and the thickness of the aluminum foil is reduced to 1.5 ⁇ m.
  • Comparative Example 3 The difference between Comparative Example 3 and Example 6 is that the width of the copper foil is the same as that of the PET, and there is no welding area.
  • Comparative Example 4 The difference between Comparative Example 4 and Example 6 is that a 4-micron-thick PE material is used as the support layer, and the thickness of the copper foil is reduced to 1 micron.
  • Comparative Example 1 Comparative Example 2, Comparative Example 2, Example 6 and Comparative Example 3 that by setting the welding area without polymer, the welding success rate of the tab can be greatly improved, and the welding success rate after welding is also guaranteed. the tensile strength of the current collector.
  • the thickness of the conductor layer is also one of the factors affecting the tab welding and the tensile strength of the current collector.
  • the influence of the conductor layer being too thin can be overcome by technical means such as setting a thickened area, expanding the scope of the thickening area, or filling conductive glue. , to improve the success rate of tab welding and the tensile strength of the current collector.
  • the current collectors prepared in the above Examples 1-10 and Comparative Examples 1-4 were made into batteries, and the failure ratio of the vibration test and the failure ratio of 300 cycles were carried out.
  • the combination of the current collectors and the test results are shown in Table 2.
  • the failure ratio of vibration test is obtained by vibration test in 7.3 of the national standard 31241-2014;
  • the failure ratio of 300 cycles is obtained by the following methods: 1C/1C charge-discharge test is carried out under the condition of temperature of 25°C, and the number of cycles after 300 cycles is recorded. The proportion of failed batteries with no voltage output.
  • Example 11 Example 1 Example 6 10% 3%
  • Example 12 Example 2
  • Example 7 0% 0%
  • Example 13 Example 3
  • Example 8 0% 0%
  • Example 14 Example 4
  • Example 9 0% 0%
  • Example 15 Example 5
  • Example 10 0% 0%
  • Example 16 Example 1
  • Example 8 2% 0% Comparative Example 5
  • Example 1 Comparative Example 3 75% 13% Comparative Example 6
  • the failure ratio of the vibration test and the failure ratio of 300 cycles of the battery made of the composite current collector in the related art are significantly higher than those of the composite current collector described in this application.
  • the fabricated batteries illustrate that the composite current collectors described in this application can be used in secondary batteries and can greatly improve the safety performance and service life of the secondary batteries.

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  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
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  • General Chemical & Material Sciences (AREA)
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Abstract

一种复合集流体。所述的复合集流体包括：支撑体层（1），该支撑体层（1）采用聚合物制成；第一导体层（2），该第一导体层（2）设置在支撑体层（1）的第一侧；第二导体层（3），该第二导体层（3）设置在支撑体层（1）的第二侧；焊接区域（4）；其中，在该焊接区域（4）内，第一导体层（2）和第二导体层（3）之间没有聚合物。

Description

一种复合集流体、制备方法及锂离子电池
本申请要求在2020年9月30日提交中国专利局、申请号为202011058984.0的中国专利申请的优先权，该申请的全部内容通过引用结合在本申请中。
技术领域
本申请涉及二次电池技术领域，例如涉及到一种复合集流体、制备方法及锂离子电池。
背景技术
锂离子电池由基本单元结构卷绕或者叠加构成，基本单元结构为正极/隔膜/负极。其中正极和负极是发生电化学反应的地方，通过正极和负极中的集流体，将电化学反应生成的电流收集并导出；隔膜负责将正极和负极分隔开，避免正负极发生接触出现短路。
集流体常见的配置方式是，负极使用铜箔材料，正极使用铝箔材料。由于使用金属材料的缘故，正负极集流体在电芯全重中占据较大的比例(8％左右)，因此降低集流体的重量是一个提高锂离子电池能量密度(kWh/kg)的有效做法，中国专利申请CN106654285A、CN101071860A通过在柔性基底表面制备导电镀层的方法，可以制备低密度集流体。还例如公布号为CN110277532A的中国专利申请，公开了一种二次电池集流体的加工方法及加工设备，通过箔材与复合集流体的转接，箔材作为复合集流体的极耳，从而能够将电芯中的电流输送出来。但是上述技术方案的缺点在于：1、极耳只与一侧的金属导体层连接，难以实现两侧的金属导体层都能将电流导出；2、由于复合集流体两侧的金属导体层通常较薄，因此很难进行焊接。
申请公布号CN110165223A的申请公开了一种复合集流体，具有多孔结构，在孔的内部具有导体层，可以实现复合集流体两侧的金属导体层导通。然而这种集流体需要进行打孔，且孔内部的导体层制作困难，导通效果差，不利于复合集流体的推广应用。授权公告号CN208051145U的实用新型公开了一种超声波焊头及焊接设备。通过焊头的锥形结构在焊接时的挤出作用，穿透焊接区域的聚合物层，将焊接区域的金属导体层焊接在一起，实现焊接的同时实现两层 金属导体层互相导通。然而这种焊接过程很容易导致过焊，破坏焊接区域的金属导体层，焊接强度低，导电能力差。
发明内容
以下是对本文详细描述的主题的概述。本概述并非是为了限制权利要求的保护范围。
本申请提供一种复合集流体，改善相关技术中复合集流体的极耳焊接困难的情况，同时改善复合集流体两侧导体层难以实现导通的情况。
本申请实施例采用以下技术方案：一种复合集流体，包括：支撑体层，该支撑体层采用聚合物制成；第一导体层，该第一导体层设置在支撑体层的一侧；第二导体层，该第二导体层设置在支撑体层的另一侧；焊接区域；其中，在该焊接区域内，第一导体层和第二导体层之间没有聚合物。
本申请实施例还公开了一种复合集流体的制备方法，用于制备如前所述的复合集流体，所述集流体包括导体层和支撑体层，包括以下步骤：将导体层材料压制成所述导体层，并将所述导体层复合在支撑体层的第一侧和第二侧。
本申请实施例还公开了一种锂离子电池，包括正极极片、负极极片、隔膜和电解质，其中，正极极片和/或负极极片包括如上所述的复合集流体。
在阅读并理解了附图和详细描述后，可以明白其他方面。
附图说明
下面结合附图和实施例对本申请进一步说明。
图1是本申请一种实施方式中的复合集流体的结构示意图。
图2是图1所示的复合集流体的俯视图。
图3A是本申请另一种实施方式中的复合集流体的结构示意图。
图3是图3A所示的复合集流体的俯视图。
图4是本申请第三种实施方式中的复合集流体的结构示意图。
图5是本申请第四种实施方式中的复合集流体的结构示意图。
图6是本申请第五种实施方式中的复合集流体的结构示意图。
附图中
1、支撑体层 2、第一导体层 3、第二导体层
4、焊接区域 5、导电胶
具体实施方式
以下结合附图对本申请实施例进行详细说明。应当理解，此处所描述的示例实施例是本申请一部分实施例，而不是全部的实施例，仅仅用以解释本申请实施例，并不用于限定本申请实施例，本领域普通技术人员在没有做出创造性劳动前提下所获得的所有其他实施例，都属于本申请保护的范围。
在本申请的描述中，需要说明的是，术语“中心”、“中”、“上”、“下”、“左”、“右”、“内”、“外”、“顶”、“底”、“侧”、“竖直”、“水平”等指示的方位或位置关系为基于附图所示的方位或位置关系，仅是为了便于描述本申请和简化描述，而不是指示或暗示所指的装置或元件必须具有特定的方位、以特定的方位构造和操作，因此不能理解为对本申请的限制。此外，术语“一”、“第一”、“第二”、“第三”、“第四”、“第五”、“第六”仅用于描述目的，而不能理解为指示或暗示相对重要性。
在本申请的描述中，需要说明的是，除非另有明确的规定和限定，术语“安装”、“相连”、“连接”应做广义理解，例如，可以是固定连接，也可以是可拆卸连接，或一体地连接；可以是机械连接，也可以是电连接；可以是直接相连，也可以通过中间媒介间接相连，可以是两个元件内部的连通。对于本领域的普通技术人员而言，可以具体情况理解上述术语在本申请中的具体含义。
出于简明和说明的目的，实施例的原理主要通过参考例子来描述。在以下描述中，很多具体细节被提出用以提供对实施例的彻底理解。然而明显的是，对于本领域普通技术人员，这些实施例在实践中可以不限于这些具体细节。在一些实例中，没有详细地描述公知方法和结构，以避免无必要地使这些实施例变得难以理解。另外，所有实施例可以互相结合使用。
本申请通过图1显示了一种复合集流体的结构示意图，图2为图1所示的复合集流体的俯视图。如图1-2所示，所述的复合集流体包括支撑体层1、第一导体层2和第二导体层3，第一导体层2和第二导体层3分别复合在支撑体层1的两侧。其中，支撑体层1采用聚合物材料制成，用于提供支撑力。第一导体层2和第二导体层3一般采用同种导电材料，用于将电流导出。
图2中，虚线表示第一导体层2和第二导体层3与支撑体层1的相交位置，阴影线表示焊接区域4。
对此，为了改善复合集流体的极耳焊接困难的情况，上述的复合集流体还包 括至少一个焊接区域4，在该焊接区域4内，第一导体层2和第二导体层3之间没有用于制备支撑体层1的聚合物(因此图2中的焊接区域4没有延伸至虚线处)。设置没有聚合物的焊接区域4，在焊接极耳时，不需要穿透支撑体层1即可实现第一导体层2和第二导体层3之间的相互电连接，进而将第一导体层2和第二导体层3上产生的电流导出，改善相关技术中复合集流体的极耳焊接困难的情况和复合集流体两侧导体层难以实现导通的情况。
其中，支撑体层1采用的聚合物材料为聚对苯二甲酸乙二醇酯(Polyethylene terephthalate，PET)、聚丙烯(Polypropylene，PP)、聚乙烯(Polyethylene，PE)、聚酰亚胺(Polyimide，PI)、聚芳砜中的一种或多种，或者也可以采用其他质量轻、强度大的绝缘材料作为替代。在一实施例中，支撑体层1的厚度为2微米-6微米。
第一导体层2和第二导体层3可以采用铝、铜、镍、银、金、碳、不锈钢或其合金制成。在一实施例中，用作正极集流体的第一导体层2和第二导体层3一般采用铝或铝合金材料制成，而作为负极集流体的第一导体层2和第二导体层3一般采用铜或铜合金材料制成。
其中，第一导体层2和第二导体层3的厚度为0.2-5微米。若第一导体层2和第二导体层3的厚度小于0.2微米，则导电能力不足，内阻大；若厚度超过5微米，则厚度和重量过大，影响电池能量密度。
其次，在本申请中，焊接区域4的面积占第一导体层2(或第二导体层3)的面积的0.5-30％。若焊接区域4的面积占比超过30％，则第一导电层2和第二导体层3没有足够的支撑面积(支撑体层1提供的)，容易损坏。若焊接区域的面积占比小于0.5％，则不能够提供足够的面积进行焊接极耳。
其中，焊接区域4可以示例实施为矩形、圆形、椭圆形、扇形、多边形或者不规则图形等各种形状，并不限制本申请。焊接区域4也可以设置在复合集流体上的任何位置，在一实施例中可以设置在复合集流体的边缘，这样便于后续进行焊接极耳。
示例性的，如图1-2所示，W表示的方向为宽度方向，焊接区域4由第一导体层2和第二导体层3的宽度宽于支撑体层4而形成，这样可以在将第一导体层2和第二导体层3复合在支撑体层4两侧时，自然地在复合集流体的边缘形成焊接区域4，不需要对支撑体层4进行额外的操作。
图3A显示了本申请另一种实施方式中的复合集流体的结构示意图，图3是 图3A所示的复合集流体的俯视图。如图3A和图3所示，所述的焊接区域4也能够由支撑体层镂空形成。镂空区域采用图3中的阴影线表示，图中的A-A’处不存在镂空区域，B-B’处设置有镂空区域(即焊接区域4)。
图4显示了本申请第三实施方式中的复合集流体的结构。图4在图1的基础上，使焊接区域4内的第一导体层2和/或第二导体层3的厚度大于其剩余部分，形成加厚区域。在一实施例中，在第一导体层1上，焊接区域4内的加厚区域的厚度为h2，剩余部分的厚度为h1，h2>h1。这样设置，可以增强焊接区域4的强度，避免在加工过程中损坏；还可以增强焊接的第一导体层2和第二导体层3的厚度，提升焊接强度。
图5显示了本申请第四种实施方式中的复合集流体的结构。图5在图4的基础上，W表示的方向为宽度方向，加厚区域的边缘宽于焊接区域4，宽度为0.5-10mm，使得加厚区域的边缘与支撑体层1的边缘重叠，增强焊接区域4的强度，避免在焊接区域4的边缘出现导体层断裂的情况。
图6显示了本申请第五种实施方式中的复合集流体的结构。图6在图4的基础上，在焊接区域4内的第一导体层2和第二导体层3之间填充了导电胶5，通过导电胶5的粘接可以提高焊接区域4的强度，避免损坏，也能提升焊接后第一导体层2和第二导体层3的强度。
在上述技术方案中，所述的复合集流体的制备方法可以包括以下步骤：将导体层材料压制成导体层后，将导体层与支撑体层材料复合。其中，导体层与支撑体层可以通过胶粘剂连接复合。完成复合的导体层可以通过化学或者电化学方法进行减薄。
对此，若想要在复合集流体上形成上述的加厚区域，只需要在焊接区域上的导体层表面设置遮挡物，阻断在焊接区域上对导体层的腐蚀。遮挡物可以是胶带，在完成减薄后需要将该胶带去除。
在上述技术方案中，上述的复合集流体可以用于制作极片：在集流体表面涂布正极活性材料，制得正极极片；在集流体表面涂布负极活性材料，制得负极极片。以卷绕方式将正极极片、隔膜和负极极片组装形成干电芯。将干电芯装入电池壳体内并注电解液，经过充电化成，制得二次电池。
下面通过实施例对本申请进行说明，但本申请不限于这些实施例。
【实施例1】
将纯度99.7％的铝材进行轧制加工，获得5微米厚的铝箔。将5微米厚的铝箔通过胶黏剂复合在5微米厚的PET的两侧，形成正极集流体。其中PET分子量192.17，胶黏剂为无锡宇科生产的WB888胶，复合的温度为95摄氏度，复合压力0.5兆帕，复合后静置时间为150小时。5微米铝箔宽度为100mm，PET宽度为80mm。焊接区域的面积占比为20％。
采用20％NaOH溶液进行化学腐蚀，温度为45摄氏度，腐蚀时间为1分钟，然后使用去离子水冲洗烘干。上述的单侧铝层厚度经过化学腐蚀后为3微米。
【实施例2】
实施例2与实施例1的区别在于，采用4微米厚的PET材料作为支撑体层，3微米厚的铝箔为导体层；铝箔宽度为100mm，PET宽度为90mm，焊接区域的面积占比为10％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域，且加厚区域的宽度比焊接区域宽1mm。铝箔完成减薄后，加厚区域的厚度为3微米，剩余区域的厚度为2微米。
【实施例3】
实施例3与实施例1的区别在于，采用3微米厚的PP材料作为支撑体层，5微米厚的铝箔作为导体层；铝箔宽度为100mm，PET宽度为95mm，焊接区域的面积占比为5％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域。铝箔完成减薄后，加厚区域的厚度为5微米，剩余区域的厚度为2微米。
【实施例4】
实施例4与实施例1的区别在于，采用2微米厚的PE材料作为支撑体层，10微米厚的铝箔作为导体层；铝箔宽度为100mm，PET宽度为70mm，焊接区域的面积占比为30％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域。铝箔完成减薄后，加厚区域的厚度为10微米，剩余区域的厚度为5微米。此外，在焊接区域内填充导电胶。
【实施例5】
实施例5与实施例1的区别在于，采用6微米厚的PI材料作为支撑体层，2微米厚的铝箔作为导体层；铝箔宽度为100mm，PET宽度为75mm，焊接区域 的面积占比为25％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域。铝箔完成减薄后，加厚区域的厚度为2微米，剩余区域的厚度为0.5微米。此外，在焊接区域内填充导电胶。
【实施例6】
将纯度99.7％的铜进行轧制加工，获得5微米厚的铜箔。将5微米厚的铜箔通过胶黏剂复合在5微米厚的PET的两侧，形成正极集流体。其中PET分子量192.17，胶黏剂为无锡宇科生产的WB888胶，复合的温度为95摄氏度，复合压力0.5兆帕，复合后静置时间为150小时。4微米铜箔的宽度为100mm，PET宽度为80mm，焊接区域的面积占比为20％。
采用20％NaOH溶液进行化学腐蚀，温度为45摄氏度，腐蚀时间为1分钟，然后使用去离子水冲洗烘干。上述的单侧铜箔厚度经过化学腐蚀后为4微米。
【实施例7】
实施例7与实施例6之间的区别在于，采用4微米厚的PP材料作为支撑体层，6微米厚的铜箔作为导体层；铜箔的宽度为100mm，PET宽度为90mm，焊接区域的面积占比为10％；完成减薄的单侧铜箔厚度为5微米。
【实施例8】
实施例8与实施例6之间的区别在于，采用3微米厚的PET材料作为支撑体层，3微米厚的铜箔作为导体层；铜箔的宽度为100mm，PET宽度为99mm，焊接区域的面积占比为1％
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域，且加厚区域的宽度比焊接区域宽0.5mm。铝箔完成减薄后，加厚区域的厚度为3微米，剩余区域的厚度为1微米。
【实施例9】
实施例9与实施例6的区别在于，采用2微米厚的聚芳砜材料作为支撑体层，3微米厚的铜箔作为导体层；铜箔的宽度为100mm，PET宽度为85mm，焊接区域的面积占比为15％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域。铝箔完成减薄后，加厚区域的厚度为3微米，剩余区域的厚度为0.5微米。此外，在焊接区域内填充导电胶。
【实施例10】
实施例10与实施例6的区别在于，采用5微米厚的PE材料作为支撑体层，6微米厚的铜箔作为导体层；铜箔的宽度为100mm，PET宽度为70mm，焊接区域的面积占比为30％。
在采用20％NaOH溶液进行化学腐蚀减薄时，在焊接区域上的导体层表面覆盖胶带，形成加厚区域。铝箔完成减薄后，加厚区域的厚度为6微米，剩余区域的厚度为2微米。此外，在焊接区域内填充导电胶。
【对比例1】
对比例1与实施例1之间的区别在于，铝箔的宽度与PET的宽度一致，无焊接区域。
【对比例2】
对比例2与实施例1之间的区别在于，采用4微米厚的PP材料作为支撑体层，且铝箔的厚度减薄至1.5微米。
【对比例3】
对比例3与实施例6之间的区别在于，铜箔的宽度与PET的宽度一致，无焊接区域。
【对比例4】
对比例4与实施例6之间的区别在于，采用4微米厚的PE材料作为支撑体层，且铜箔的厚度减薄至1微米。
为了说明本申请技术方案的技术凉，将上述实施例及对比例中的集流体制得各300片，进行极耳的焊接，并计算焊接成功率。同时，对完成的集流体进行拉伸强度测试，测试方法采用HB 5280-1996中记载的金属箔材的拉伸强度的测试标准。测试结果如表1所示。
表1
Figure PCTCN2021092598-appb-000001
Figure PCTCN2021092598-appb-000002
如表1所示，由对比实施例1和对比例2、实施例6和对比例3可知，通过设置没有聚合物的焊接区域，能够大大提高极耳的焊接成功率，同时也保证了焊接后的集流体的拉伸强度。同时，导体层的厚度也是影响极耳焊接及集流体拉伸强度的因素之一，但可以通过设置加厚区域、扩大加厚区域的范围或填充导电胶等技术手段克服导体层过薄的影响，提高极耳焊接的成功率及集流体的拉伸强度。
下面，将上述实施例1-10及对比例1-4制得的集流体制成电池，并进行震动测试失效比例以及300次循环失效比例，集流体的组合以及测试结果如表2所示。其中，震动测试失效比例采用国标31241-2014中7.3振动测试获得；300次循环失效比例通过以下方式获得：在温度为25℃的条件下进行1C/1C充放电测试，记录经过300次循环次数下无电压输出的失效电池比例。
表2
  正极集流体 负极集流体 震动测试失效比例 300次循环失效比例
实施例11 实施例1 实施例6 10％ 3％
实施例12 实施例2 实施例7 0％ 0％
实施例13 实施例3 实施例8 0％ 0％
实施例14 实施例4 实施例9 0％ 0％
实施例15 实施例5 实施例10 0％ 0％
实施例16 实施例1 实施例8 2％ 0％
对比例5 实施例1 对比例3 75％ 13％
对比例6 实施例1 对比例4 100％ 25％
对比例7 对比例1 实施例6 75％ 11％
对比例8 对比例2 实施例6 100％ 19％
如表2所示，采用了相关技术中的复合集流体制成的电池(对比例5-8)的震动测试失效比例及300次循环失效比例均明显高于采用本申请所述的复合集流体制成的电池(实施例11-16)，说明本申请所述的复合集流体，应用于二次电池中，能够大大提高二次电池的安全性能和使用寿命。
尽管上面对本申请说明性的示例实施方式进行了描述，以便于本技术领域的技术人员能够理解本申请，但是本申请不仅限于示例实施方式的范围，对本技 术领域的普通技术人员而言，只要各种变化只要在所附的权利要求限定和确定的本申请精神和范围内，一切利用本申请构思的申请创造均在保护之列。

Claims (16)

  1. 一种复合集流体，包括：
    支撑体层，所述支撑体层采用聚合物制成；
    第一导体层，所述第一导体层设置在所述支撑体层的第一侧；
    第二导体层，所述第二导体层设置在所述支撑体层的第二侧；
    焊接区域；
    其中，在所述焊接区域内，所述第一导体层和第二导体层之间没有所述聚合物。
  2. 根据权利要求1所述的复合集流体，其中，所述支撑体层采用聚对苯二甲酸乙二醇酯PET、聚丙烯PP、聚乙烯PE、聚酰亚胺PI、聚芳砜中的一种或多种材料制成。
  3. 根据权利要求1所述的复合集流体，其中，所述第一导体层和所述第二导体层分别采用以下之一的材料：铝；铜；镍；银；金；碳；不锈钢；铝合金；铜合金；镍合金；银合金；金合金；碳合金；铝、铜、镍、银、金中的至少一种与碳的混合物；不锈钢与碳的混合物；铝合金、铜合金、镍合金、银合金、金合金中的至少一种与碳的混合物；碳合金与碳的混合物。
  4. 根据权利要求1所述的复合集流体，其中，所述第一导体层和所述第二导体层的厚度分别为0.2-5微米。
  5. 根据权利要求1所述的复合集流体，其中，所述焊接区域的面积占所述第一导体层的面积的0.5-30％。
  6. 根据权利要求1所述的复合集流体，其中，所述焊接区域的形状为矩形、圆形、椭圆形、扇形、多边形或者不规则图形。
  7. 根据权利要求1所述的复合集流体，其中，所述焊接区域位于所述复合集流体的边缘。
  8. 根据权利要求1所述的复合集流体，其中，所述焊接区域由所述第一导体层和所述第二导体层的宽度宽于所述支撑体层而形成。
  9. 根据权利要求1所述的复合集流体，其中，所述焊接区域由所述支撑体层镂空形成。
  10. 根据权利要求1所述的复合集流体，其中，在所述焊接区域中，所述第一导体层和所述第二导体层之间具有导电胶。
  11. 根据权利要求1所述的复合集流体，其中，
    所述第一导体层在所述焊接区域内的厚度大于所述第一导体层在所述焊接区域之外的厚度，以形成加厚区域；
    所述第二导体层在所述焊接区域内的厚度大于所述第二导体层在所述焊接区域之外的厚度，以形成加厚区域；
    所述第一导体层和所述第二导体层在所述焊接区域内的厚度分别大于所述第一导体层和所述第二导体层在所述焊接区域之外的厚度，以形成加厚区域。
  12. 根据权利要求11所述的复合集流体，其中，所述加厚区域的宽度比所述焊接区域的宽度大0.5-10mm。
  13. 一种复合集流体的制备方法，用于制备如权利要求1所述的复合集流体，所述集流体包括导体层和支撑体层，包括：将导体层材料压制成所述导体层，并将所述导体层复合在所述支撑体层的第一侧和第二侧。
  14. 根据权利要求13所述的方法，其中，所述导体层与所述支撑体层通过胶黏剂连接。
  15. 根据权利要求13所述的方法，其中，所述导体层通过化学或者电化学方法进行减薄。
  16. 一种锂离子电池，包括正极极片、负极极片、隔膜和电解质，其中，
    所述正极极片和所述负极极片中的至少一种包括如权利要求1-15中任一项所述的复合集流体。
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