WO2024011529A1 - Collecteur de courant composite, son procédé de préparation et son application - Google Patents

Collecteur de courant composite, son procédé de préparation et son application Download PDF

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Publication number
WO2024011529A1
WO2024011529A1 PCT/CN2022/105792 CN2022105792W WO2024011529A1 WO 2024011529 A1 WO2024011529 A1 WO 2024011529A1 CN 2022105792 W CN2022105792 W CN 2022105792W WO 2024011529 A1 WO2024011529 A1 WO 2024011529A1
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Prior art keywords
current collector
polymer material
metal layer
composite current
layer
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PCT/CN2022/105792
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English (en)
Chinese (zh)
Inventor
王成豪
李学法
张国平
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扬州纳力新材料科技有限公司
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Priority to PCT/CN2022/105792 priority Critical patent/WO2024011529A1/fr
Publication of WO2024011529A1 publication Critical patent/WO2024011529A1/fr

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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
    • 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
    • H01M4/80—Porous plates, e.g. sintered carriers
    • 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

Definitions

  • the present invention relates to the field of battery technology, and specifically to a composite current collector and its preparation method and application.
  • the current metal composite current collectors are mainly copper current collectors or aluminum current collectors.
  • the copper current collector or aluminum current collector is composed of two parts, including a metal layer and a polymer layer located between the metal layers.
  • the polymer layer in the middle of a conventional metal composite current collector has a non-porous structure, that is, the porosity is 0, and the upper and lower metal layers cannot conduct the ions above and below the current collector, resulting in the resistivity of the upper and lower metal layers. There is a difference, and the ion field formed is uneven, which leads to greater internal polarization of the battery and affects the electrochemical performance of the battery.
  • the present invention provides a composite current collector, which includes a first metal layer, a second metal layer and a polymer material layer.
  • the polymer material layer is located between the first metal layer and the second metal layer.
  • the composite current collector has a through-hole structure penetrating the first metal layer, the second metal layer and the polymer material layer; the pore diameter of the through-hole structure is 0.1 mm ⁇ 1 mm, and the porosity 0.1% to 5%.
  • the pore diameter of the through-hole structure is 0.5 mm to 1 mm, and the porosity is 0.1% to 5%.
  • the thickness of the composite current collector is 2 ⁇ m ⁇ 28 ⁇ m, wherein the thickness of the first metal layer and the second metal layer may be independently 0.5 ⁇ m ⁇ 1.5 ⁇ m, and the polymer material The thickness of the layer may range from 1 ⁇ m to 25 ⁇ m.
  • the material of the polymer material layer is selected from the group consisting of a composite of an insulating polymer material and an inorganic non-conductive filler, a composite of an insulating polymer material and a conductive filler, an insulating polymer material or a conductive polymer.
  • the insulating polymer material is selected from the group consisting of cellulose and its derivatives, starch and its derivatives, proteins and its derivatives, polyvinyl alcohol and its cross-linked polymers, polyethylene glycol and its cross-linked polymers.
  • copolymer polyamide, polyterephthalate, polyimide, polyethylene, polypropylene, polystyrene, polyvinyl chloride, aramid, polyphenylenediamide, acrylonitrile-butadiene Olefin-styrene copolymer, polyethylene terephthalate, polybutylene terephthalate, poly(p-phenylene terephthalamide), polypropylene, polyformaldehyde, epoxy resin, phenolic resin , one or more of polytetrafluoroethylene, polyvinylidene fluoride, silicone rubber and polycarbonate; and/or
  • the conductive polymer material is selected from doped polysulfide nitride and/or doped polyacetylene; and/or
  • the inorganic non-conductive filler is selected from one or more of ceramic materials, glass materials and ceramic composite materials; and/or
  • the conductive filler is selected from one or more of carbon black, carbon nanotubes, graphite, acetylene black, graphene, nickel, iron, copper, aluminum, alloy, nickel-coated graphite powder and nickel-coated carbon fiber. .
  • the present invention also provides a method for preparing the composite current collector as described above, which includes the following steps:
  • the first metal layer and the second metal layer are respectively formed on both sides of the polymer material layer, and holes are drilled through the polymer material layer and the first metal layer according to the distribution principle of the through-hole structure. layer and the second metal layer.
  • the plating method is vacuum evaporation, and/or the drilling method is laser drilling;
  • the evaporation temperature of the plating material for vacuum evaporation is 600°C to 1600°C, the vacuum degree is ⁇ 1 ⁇ 10 -2 Pa, and the evaporation rate is 10m/min to 100m/min;
  • the wavelength of the laser drilling is 400nm ⁇ 700nm.
  • the present invention further provides a cathode, which includes the above-mentioned composite current collector and a cathode active material layer located on the surface of the composite current collector.
  • the present invention provides a battery, which includes the above-mentioned positive electrode.
  • the present invention also provides an electrical device, which includes the above-mentioned battery.
  • a porous composite current collector is prepared by arranging through holes and regulating the diameter and distance of the through holes.
  • the through-hole structure can allow ions to pass through, so that the ion concentrations on the surfaces of the first metal layer and the second metal layer gradually tend to Consistently, the polarization on the surface of the first metal layer and the second metal layer of the composite current collector is reduced, and the electrical performance of the battery is improved, especially while reducing the internal resistance of the battery and improving its rate performance.
  • Figure 1 is a schematic structural diagram of a porous composite current collector produced in one embodiment of the present invention
  • Figure 2 is a top view of the porous composite current collector in Figure 1.
  • the first object of the present invention is to provide a composite current collector, which includes a first metal layer, a second metal layer and a polymer material layer.
  • the polymer material layer is located between the first metal layer and the second metal layer.
  • the composite current collector It has a through-hole structure penetrating the first metal layer, the second metal layer and the polymer material layer; wherein the through-hole structure has a pore diameter of 0.1 mm to 1 mm and a porosity of 0.1% to 5%.
  • a porous composite current collector is prepared by arranging through holes and regulating the diameter and distance of the through holes.
  • the through-hole structure can allow ions to pass through, so that the ion concentrations on the surfaces of the first metal layer and the second metal layer tend to be consistent.
  • the polarization on the surface of the first metal layer and the second metal layer of the composite current collector is reduced, thereby improving the electrical performance of the battery, especially while reducing the internal resistance of the battery and improving its rate performance.
  • the aperture of the through-hole structure can be any value between 0.1mm and 1mm, preferably between 0.5mm and 1mm.
  • it can also be 0.6mm, 0.7mm, 0.8mm, 0.9mm;
  • the porosity can be any value between 0.1% and 5%, for example, it can also be 0.5%, 1%, 2%, 3%, 4%, or 4.5%.
  • the center distance between two adjacent through holes can be any value between 5mm and 10mm, for example, it can also be 5.5mm, 6mm, 6.5mm, 7mm, 7.5mm, 8mm, 8.5 mm, 9mm, 9.5mm, preferably any value between 8mm and 10mm.
  • the thickness of the composite current collector may be 2 ⁇ m to 28 ⁇ m, for example, it may also be 5 ⁇ m, 8 ⁇ m, 10 ⁇ m, 12 ⁇ m, 15 ⁇ m, 18 ⁇ m, 20 ⁇ m, 22 ⁇ m, or 25 ⁇ m.
  • the thickness of the first metal layer and the second metal layer may be independently 0.5 ⁇ m to 1.5 ⁇ m, and the thickness of the polymer material layer may be 1 ⁇ m to 25 ⁇ m.
  • the polymer material layer can be made of any material commonly used in the art, including but not limited to a composite of insulating polymer materials and inorganic non-conductive fillers, or a composite of insulating polymer materials and conductive fillers. material, insulating polymer material or conductive polymer material, wherein the mass percentage of insulating polymer material in the composite formed by insulating polymer material and inorganic non-conductive filler is ⁇ 90%, and the composite formed by insulating polymer material and conductive filler The mass percentage of medium insulating polymer material is ⁇ 90%.
  • the insulating polymer material may be selected from the group consisting of cellulose and its derivatives, starch and its derivatives, protein and its derivatives, polyvinyl alcohol and its cross-linked polymers, polyethylene glycol and its cross-linked polymers, polyethylene glycol and its cross-linked polymers.
  • the conductive polymer material may be selected from doped polysulfide nitride and/or doped polyacetylene.
  • the inorganic non-conductive filler can be selected from one or more of ceramic materials, glass materials and ceramic composite materials;
  • the conductive filler can be selected from at least one of conductive carbon materials, metal materials, and composite conductive materials.
  • the carbon material can be selected from carbon black, carbon nanotubes, graphite, acetylene black, and graphene.
  • the metal material can be selected from Nickel, iron, copper, aluminum, alloy, wherein the alloy contains one or more of nickel, iron, copper and aluminum, the composite conductive material can be selected from one of nickel-coated graphite powder and nickel-coated carbon fiber or more.
  • the puncture strength of the polymer material layer is ⁇ 100gf
  • the longitudinal (MD) tensile strength is ⁇ 180MPa
  • the longitudinal (MD) elongation is ⁇ 10%
  • the transverse (TD) tensile strength is ⁇ 180MPa
  • the transverse (TD) tensile strength is ⁇ 180MPa.
  • the composite current collector is a positive electrode current collector, and its puncture strength is ⁇ 50gf, the longitudinal (MD) tensile strength is ⁇ 180MPa, the longitudinal (MD) elongation is ⁇ 10%, and the transverse (TD) tensile strength is ⁇ 180MPa. , Transverse (TD) elongation ⁇ 10%.
  • the peeling force between the first metal layer and the second metal layer and the polymer material layer is ⁇ 5 N/m.
  • the first metal layer and the second metal layer may be copper metal layers or aluminum metal layers.
  • the purity of the first metal layer and the second metal layer is ⁇ 99.8%.
  • the present invention also provides a method for preparing the composite current collector as described above, which includes the following steps:
  • a first metal layer and a second metal layer are respectively formed on both sides of the polymer material layer, and holes are drilled through the polymer material layer, the first metal layer and the second metal layer according to the distribution principle of the through-hole structure.
  • the plating method can be vacuum evaporation, where the parameters of vacuum evaporation need to meet any of the following: the evaporation temperature of the plating material can be 600°C to 1600°C, and the vacuum degree is ⁇ 1 ⁇ 10 -2 Pa, the evaporation rate is 10m/min ⁇ 100m/min.
  • the degree of vacuum may be 0.1 ⁇ 10 -2 Pa to 0.8 ⁇ 10 -2 Pa.
  • the evaporation rate is the moving speed of the polymer material layer.
  • the drilling method may be laser drilling; preferably, the wavelength of laser drilling may be 400 nm to 700 nm.
  • the preparation method further includes the steps of rolling and vacuum packaging.
  • the present invention further provides a cathode, which includes the above-mentioned composite current collector and a cathode active material layer located on the surface of the composite current collector.
  • the cathode active material in the cathode active material layer can be any cathode active material known in the art, for example, it can be lithium cobalt oxide, lithium iron phosphate, NCA, NCM, lithium manganate, lithium nickelate , NCMA or cobalt-free cathode.
  • the present invention provides a battery, which includes the above-mentioned positive electrode.
  • the battery may further include a negative electrode and an electrolyte.
  • the negative electrode can also be any negative electrode commonly used in this field, such as graphite, lithium, and lithium titanate.
  • the electrolyte may be a solid electrolyte, a semi-solid electrolyte or a liquid electrolyte, wherein the solid electrolyte and the semi-solid electrolyte may be oxide or sulfide electrolytes, and the solute in the liquid electrolyte may be lithium hexafluorophosphate.
  • the battery may further include a separator, wherein the separator may be any separator known in the art, such as a PE wet separator, a PP dry separator or a double-layer PE/PP coated separator.
  • the separator may be any separator known in the art, such as a PE wet separator, a PP dry separator or a double-layer PE/PP coated separator.
  • the shape of the battery is not limited, for example, it can be cylindrical, square, or can also be an aluminum-plastic film soft package.
  • the battery may be a lithium-ion battery.
  • the present invention also provides an electrical device, which includes the above-mentioned battery.
  • specific types of electrical devices include, but are not limited to, mobile terminals (mobile phones, mobile computers, etc.), smart wearables, power tools (electric drills, electric motors, etc.), electric vehicles, mobile power supplies, etc.
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a PET film
  • the pore structure runs through the thickness direction of the porous composite current collector.
  • Channel 400 is formed.
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to obtain a porous composite current collector with channels 400; wherein the depth of the channels 400 is 8 ⁇ m and the pore diameter is 0.5 mm. The center distance between adjacent circular holes is 8mm; the wavelength of laser drilling is 600nm.
  • the measured puncture strength of the porous composite current collector is 200gf; the longitudinal (MD) tensile strength is 210MPa, and the longitudinal (MD) elongation is 35%; the transverse (TD) tensile strength is 190MPa, and the transverse (TD) elongation is 15 %.
  • the peeling force between the first metal layer 100 or the second metal layer 200 and the polymer material layer 300 was measured to be 5 N/m.
  • Positive electrode composed of the porous composite current collector prepared in (1) and the lithium iron phosphate active material coated on the porous composite current collector;
  • Negative electrode graphite
  • Electrolyte liquid electrolyte with lithium hexafluorophosphate as solute
  • the method of preparing the porous composite current collector in this embodiment is basically the same as that in Example 1, except that the pore diameter is 1 mm. Specific steps are as follows:
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a PET film
  • the pore structure runs through the thickness direction of the porous composite current collector.
  • Channel 400 is formed.
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to prepare a porous composite current collector; wherein, the depth of the hole channel 400 is 8 ⁇ m, the aperture is 1 mm, and the adjacent circular holes are The center distance between the circles is 8mm; the wavelength of laser drilling is 600nm.
  • the method of preparing the porous composite current collector in this embodiment is basically the same as that in Embodiment 1, except that the center distance between adjacent circular holes is 5 mm. Specific steps are as follows:
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a PET film
  • the pore structure runs through the thickness direction of the porous composite current collector.
  • Channel 400 is formed.
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to prepare a porous composite current collector; wherein the depth of the hole channel 400 is 8 ⁇ m, the aperture is 0.5 mm, and the adjacent circular holes are The center distance between the circles is 5mm; the wavelength of laser drilling is 500nm.
  • the method of preparing the porous composite current collector in this embodiment is basically the same as that in Embodiment 1, except that the center distance between adjacent circular holes is 10 mm. Specific steps are as follows:
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a PET film
  • the pore structure runs through the thickness direction of the porous composite current collector.
  • Channel 400 is formed.
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to prepare a porous composite current collector; wherein the depth of the hole channel 400 is 8 ⁇ m, the aperture is 0.5 mm, and the adjacent circular holes are The center distance between the circles is 10mm; the wavelength of laser drilling is 600nm.
  • the method of preparing the porous composite current collector in this embodiment is basically the same as that in Embodiment 1, except that the polymer material layer 300 is made of a conductive film composed of polyethylene and graphite with a mass ratio of 9:1. Specific steps are as follows:
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a conductive material composed of polyethylene and graphite (mass ratio is 9:1).
  • the film and pore structure run through the thickness direction of the porous composite current collector to form pore channels 400 .
  • the specific preparation steps are as follows:
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to prepare a porous composite current collector; wherein the depth of the hole channel 400 is 8 ⁇ m, the aperture is 0.5 mm, and the adjacent circular holes are The center distance between the circles is 8mm; the parameters of laser drilling are as follows: the wavelength is 600nm.
  • the preparation method of this comparative example is basically the same as that of Example 1, except that the current collector is not perforated, that is, the holes 400 are not formed. Specific steps are as follows:
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • the puncture strength of the composite current collector was measured to be 190gf; the longitudinal (MD) tensile strength was 220MPa, and the longitudinal (MD) elongation was 43%; the transverse (TD) tensile strength was 200MPa, and the transverse (TD) elongation was 21% .
  • the peeling force between the first metal layer 100 or the second metal layer 200 and the polymer material layer 300 was measured to be 5 N/m.
  • Positive electrode composed of the composite current collector prepared in (1) and the lithium iron phosphate active material coated on the composite current collector;
  • Negative electrode graphite
  • Electrolyte liquid electrolyte with lithium hexafluorophosphate as solute
  • the preparation method of this comparative example is basically the same as that of Example 1, except that the hole diameter is 2 mm. Specific steps are as follows:
  • the first metal layer 100 and the second metal layer 200 are both metal aluminum layers
  • the polymer material layer 300 is a PET film
  • the pore structure runs through the thickness direction of the porous composite current collector.
  • Channel 400 is formed.
  • the specific parameters are as follows: vacuum degree is 0.5 ⁇ 10 -2 Pa, plating material temperature is 650°C, and evaporation rate is 100m/min.
  • step 2) Use laser drilling to drill holes in the thickness direction of the composite current collector prepared in step 1) to obtain a porous composite current collector with pore channels 400; wherein the depth of the pore channels 400 is 8 ⁇ m and the pore diameter is 2 mm. The center distance between adjacent circular holes is 8mm; the parameters of laser drilling are as follows: the wavelength is 600nm.
  • Positive electrode composed of the porous composite current collector prepared in (1) and the lithium iron phosphate active material coated on the porous composite current collector;
  • Negative electrode graphite
  • Electrolyte liquid electrolyte with lithium hexafluorophosphate as solute
  • the polarization internal resistance test, capacity retention rate and charge and discharge cycle performance test refer to the national standard GB18287_2000, and the test results are shown in Table 1.
  • Capacity retention rate Test the capacity retention rate of the lithium iron phosphate batteries assembled in Example 1 and Comparative Examples 1-2 at 25°C and 3C rate for 1000 cycles. The test results are shown in Table 1;
  • the ion concentration of the upper and lower metal layers of the current collector can be made consistent, thereby reducing the polarization on the surface of the upper and lower metal layers of the porous composite current collector, and improving the performance of the battery. Electrical properties, especially the internal resistance and rate performance of the battery. Furthermore, further regulating the parameters of the pore structure, such as the pore diameter and the center distance between the pores, can reduce the polarization of the porous composite current collector while having excellent mechanical strength. Moreover, larger pore diameter and more pores will also reduce the strength of the composite current collector.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Cell Electrode Carriers And Collectors (AREA)

Abstract

L'invention concerne un collecteur de courant composite, son procédé de préparation et son application. Le collecteur de courant composite comprend une première couche métallique (100), une seconde couche métallique (200) et une couche de matériau polymère (300). La couche de matériau polymère (300) est située entre la première couche métallique (100) et la seconde couche métallique (200). Le collecteur de courant composite présente une structure de trou traversant passant à travers la première couche métallique (100), la seconde couche métallique (200) et la couche de matériau polymère (300). Le diamètre de pore de la structure de trou traversant est de 0,1 à 1 mm, et la porosité est de 0,1 à 5 %. Selon le collecteur de courant composite, une conduction ionique peut être mise en œuvre, une polarisation dans les batteries peut être réduite, et les performances électrochimiques de batteries peuvent être améliorées.
PCT/CN2022/105792 2022-07-14 2022-07-14 Collecteur de courant composite, son procédé de préparation et son application WO2024011529A1 (fr)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20120315537A1 (en) * 2011-06-10 2012-12-13 Yardney Technical Products Inc. Composite current collector, methods of manufacture thereof, and articles including the same
CN108281662A (zh) * 2017-01-12 2018-07-13 宁德时代新能源科技股份有限公司 一种集流体，其极片和电池及应用
CN109994740A (zh) * 2019-03-29 2019-07-09 宁德新能源科技有限公司 复合集流体与包含其的复合极片及电化学装置
CN110247056A (zh) * 2018-03-30 2019-09-17 宁德时代新能源科技股份有限公司 一种集流体，其极片和电化学装置

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20120315537A1 (en) * 2011-06-10 2012-12-13 Yardney Technical Products Inc. Composite current collector, methods of manufacture thereof, and articles including the same
CN108281662A (zh) * 2017-01-12 2018-07-13 宁德时代新能源科技股份有限公司 一种集流体，其极片和电池及应用
CN110247056A (zh) * 2018-03-30 2019-09-17 宁德时代新能源科技股份有限公司 一种集流体，其极片和电化学装置
CN109994740A (zh) * 2019-03-29 2019-07-09 宁德新能源科技有限公司 复合集流体与包含其的复合极片及电化学装置

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