WO2024065161A1 - 粘结剂组合物和包含其的隔离膜 - Google Patents

粘结剂组合物和包含其的隔离膜 Download PDF

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WO2024065161A1
WO2024065161A1 PCT/CN2022/121639 CN2022121639W WO2024065161A1 WO 2024065161 A1 WO2024065161 A1 WO 2024065161A1 CN 2022121639 W CN2022121639 W CN 2022121639W WO 2024065161 A1 WO2024065161 A1 WO 2024065161A1
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Prior art keywords
monomer
acrylate
binder composition
polymer
composition according
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PCT/CN2022/121639
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English (en)
French (fr)
Chinese (zh)
Inventor
李雷
康海杨
孙成栋
郑义
艾少华
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Contemporary Amperex Technology Co Ltd
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Contemporary Amperex Technology Co Ltd
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Priority to CN202280085727.7A priority Critical patent/CN118541441A/zh
Priority to PCT/CN2022/121639 priority patent/WO2024065161A1/zh
Priority to KR1020237038040A priority patent/KR102658573B1/ko
Priority to EP22942941.0A priority patent/EP4372049A4/en
Priority to JP2023568164A priority patent/JP7763857B2/ja
Publication of WO2024065161A1 publication Critical patent/WO2024065161A1/zh
Priority to US18/765,315 priority patent/US12297305B2/en
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    • 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 field of lithium battery technology, and in particular to a binder composition and a separator containing the same.
  • the present application also relates to a secondary battery, a battery module, a battery pack and an electrical device.
  • secondary batteries are widely used in energy storage power systems such as hydropower, thermal power, wind power and solar power stations, as well as power tools, electric bicycles, electric motorcycles, electric vehicles, military equipment, aerospace and other fields.
  • energy storage power systems such as hydropower, thermal power, wind power and solar power stations, as well as power tools, electric bicycles, electric motorcycles, electric vehicles, military equipment, aerospace and other fields.
  • binders are often used in the separator of secondary batteries.
  • the existing binders have poor viscosity and are easy to cause pore blocking in the substrate, resulting in a lower porosity of the separator, a worse flow of ions in the separator, and an increase in the resistance in the separator, which affects the cycle performance of the secondary battery.
  • the present application provides a binder composition, and a separator, a secondary battery, a battery pack and an electrical device comprising the composition.
  • the first aspect of the present application provides a binder composition, comprising a polymer and ceramic particles; the polymer comprises a structural unit derived from a first monomer, a second monomer and a third monomer, and the molar ratio of the first monomer, the second monomer and the third monomer is 50 to 58:40 to 44:2 to 6;
  • the first type of monomer is selected from one or more compounds of formula I:
  • R1 is selected from hydrogen atom and straight or branched C1-6 alkyl
  • R2 is selected from substituted or unsubstituted straight or branched C1-15 alkyl, C3-6 cycloalkyl and isobornyl, and in the case of substitution, the substituent is selected from hydroxyl and C1-6 alkyl;
  • the second monomer is selected from one or more compounds of formula II:
  • R 3 is selected from a hydrogen atom and a linear or branched C1-6 alkyl group
  • the third monomer is selected from one or more compounds of formula III:
  • R4 is selected from hydrogen atom and linear or branched C1-6 alkyl
  • R5 is selected from hydrogen atom, hydroxy C1-6 alkyl and C1-6 alkoxy.
  • the adhesive composition of the present application has good bonding effect, and can increase the porosity of the isolation membrane, improve the ion conductivity, reduce the internal resistance of the isolation membrane, and improve the cycle performance of the secondary battery.
  • R1 is selected from hydrogen atom and methyl
  • R2 is selected from substituted or unsubstituted linear or branched C1-6 alkyl, in the case of substitution, the substituent is hydroxyl
  • R3 is selected from hydrogen atom and methyl
  • R4 is selected from hydrogen atom and methyl
  • R5 is selected from hydrogen atom, hydroxy C1-4 alkyl and C1-4 alkoxy.
  • the first type of monomer is selected from one or more of methyl acrylate, ethyl acrylate, n-butyl acrylate, isobutyl acrylate, sec-butyl acrylate, tert-butyl acrylate, n-propyl acrylate, cyclohexyl acrylate, lauryl acrylate, 2-ethylhexyl acrylate, 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, methyl methacrylate, ethyl methacrylate, n-butyl methacrylate, 2-ethylhexyl methacrylate, isobornyl methacrylate, lauryl methacrylate, 2-hydroxyethyl methacrylate, and 2-hydroxypropyl methacrylate; and/or the second type of monomer is acrylonitrile or methacrylonitrile; and/or the third type of monomer is selected from one or more of acrylamide
  • first, second and/or third monomers respectively helps to improve the ionic conductivity of the isolation membrane and increase the cycle capacity retention rate of the battery.
  • the molar ratio of the first monomer, the second monomer and the third monomer is 50 to 57: 41 to 44: 2 to 6.
  • the molar ratio within the above range is more conducive to the binder composition further improving the ionic conductivity of the separator and improving the cycle capacity retention rate of the battery.
  • the weight ratio of the polymer to the ceramic particles is 40 to 90: 10 to 60, and optionally 50 to 80: 20 to 50.
  • the weight ratio of the polymer to the ceramic particles is within the above range, the bonding effect of the binder with the isolation membrane and the electrode piece can be ensured, and the isolation membrane can have appropriate porosity and good ionic conductivity.
  • the weight average molecular weight of the polymer is 60000 to 120000, optionally 63300 to 118800.
  • the weight average molecular weight of the polymer is within the above range, so that the binder composition of the present application can have appropriate fluidity when bonding, thereby achieving a good bonding effect, thereby improving the cycle performance of the secondary battery.
  • the average particle size Dv50 of the ceramic particles is 40 nm to 110 nm, optionally 45 nm to 106 nm, more optionally 50 nm to 100 nm, and even more optionally 56 nm to 89 nm. Further controlling the average particle size of the ceramic particles can further improve the ionic conductivity and capacity retention rate.
  • the ceramic particles are porous particles, and the average pore size of the porous particles is 0.3nm to 6.0nm, optionally 0.5nm to 5.7nm, more optionally 1.0nm to 5.0nm, and more optionally 1.3nm to 3.8nm. Selecting porous particle materials and controlling their average pore size is conducive to further improving the porosity and ionic conductivity of the separator while ensuring the thermal stability of the separator, as well as the cycle capacity retention rate of the secondary battery.
  • the ceramic particles are porous silica particles.
  • the use of porous silica particles can further increase the porosity and ion conductivity of the separator, reduce the internal resistance of the separator, and improve the cycle performance of the secondary battery.
  • the polymer is coated on the ceramic particles, which helps to ensure that the binder composition can be evenly applied to the substrate in an ideal ratio to achieve improved heat resistance, porosity and good bonding effect.
  • the second aspect of the present application provides a separator, the separator comprising a base layer and a coating layer disposed on at least one surface of the base layer, the coating layer comprising the binder composition of the first aspect of the present application.
  • the separator of the present application can be stably bonded to the pole piece, has an increased porosity, improves ion conductivity, reduces the internal resistance of the separator, and improves the cycle performance of the secondary battery.
  • a third aspect of the present application provides a secondary battery, comprising the adhesive according to the first aspect of the present application, and/or the isolation film according to the second aspect of the present application.
  • a fourth aspect of the present application provides a battery module, comprising the secondary battery of the third aspect of the present application.
  • the fifth aspect of the present application provides a battery pack, comprising the battery module of the fourth aspect of the present application.
  • the sixth aspect of the present application provides an electrical device comprising at least one selected from the secondary battery of the third aspect of the present application, the battery module of the fourth aspect of the present application, or the battery pack of the fifth aspect of the present application.
  • the adhesive of the present application has good bonding properties, and can also increase the porosity of the isolation membrane, reduce the internal resistance of the isolation membrane, and improve the cycle performance of the secondary battery.
  • FIG. 1 is a schematic diagram of a secondary battery according to an embodiment of the present application.
  • FIG. 2 is an exploded view of the secondary battery according to the embodiment of the present application shown in FIG. 1 .
  • FIG. 3 is a schematic diagram of a battery module according to an embodiment of the present application.
  • FIG. 4 is a schematic diagram of a battery pack according to an embodiment of the present application.
  • FIG. 5 is an exploded view of the battery pack shown in FIG. 4 according to an embodiment of the present application.
  • FIG. 6 is a schematic diagram of an electric device using a secondary battery as a power source according to an embodiment of the present application.
  • range disclosed in the present application is defined in the form of a lower limit and an upper limit, and a given range is defined by selecting a lower limit and an upper limit, and the selected lower limit and upper limit define the boundaries of a particular range.
  • the range defined in this way can be inclusive or exclusive of end values, and can be arbitrarily combined, that is, any lower limit can be combined with any upper limit to form a range. For example, if a range of 60-120 and 80-110 is listed for a specific parameter, it is understood that the range of 60-110 and 80-120 is also expected.
  • the numerical range "a-b" represents the abbreviation of any real number combination between a and b, wherein a and b are real numbers.
  • the numerical range "0-5" represents that all real numbers between "0-5" have been fully listed herein, and "0-5" is just an abbreviation of these numerical combinations.
  • a parameter is expressed as an integer ⁇ 2, it is equivalent to disclosing that the parameter is, for example, an integer of 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, etc.
  • the method includes steps (a) and (b), which means that the method may include steps (a) and (b) performed sequentially, or may include steps (b) and (a) performed sequentially.
  • the method may further include step (c), which means that step (c) may be added to the method in any order.
  • the method may include steps (a), (b) and (c), or may include steps (a), (c) and (b), or may include steps (c), (a) and (b), etc.
  • the “include” and “comprising” mentioned in this application represent open-ended or closed-ended expressions.
  • the “include” and “comprising” may represent that other components not listed may also be included or only the listed components may be included or only the listed components may be included.
  • the term "or” is inclusive.
  • the phrase “A or B” means “A, B, or both A and B”. More specifically, any of the following conditions satisfies the condition "A or B”: A is true (or exists) and B is false (or does not exist); A is false (or does not exist) and B is true (or exists); or both A and B are true (or exist).
  • secondary batteries are widely used in energy storage power systems such as hydropower, thermal power, wind power and solar power stations, as well as power tools, electric bicycles, electric motorcycles, electric vehicles, military equipment, aerospace and other fields.
  • energy storage power systems such as hydropower, thermal power, wind power and solar power stations, as well as power tools, electric bicycles, electric motorcycles, electric vehicles, military equipment, aerospace and other fields.
  • secondary batteries have made great progress, higher requirements have been put forward for their energy density, cycle performance and safety performance.
  • the separator naturally becomes one of the focuses of attention of technicians.
  • ceramic particles for example, inorganic oxide particles such as silica, alumina, boehmite, etc.
  • a binder is applied to the separator coated with ceramic particles and bonded to the pole piece to prepare a secondary battery.
  • this method has its defects. First, the ceramic particles are easy to fall into the pores of the substrate and reduce the porosity of the separator, which is not conducive to ion movement; secondly, the bonding effect of the existing binder is poor.
  • the present application proposes a binder composition, which includes a polymer that plays a bonding role and ceramic particles that improve safety performance, which reduces or even avoids the occurrence of pore blocking and achieves a good bonding effect.
  • the polymer in the binder composition of the present application also helps to improve ionic conductivity due to the selection and proportion control of its monomers.
  • the binder composition of the present application can increase the porosity of the isolation membrane, increase the ionic conductivity, and improve the cycle performance of the secondary battery.
  • the present application provides a binder composition, which includes a polymer and ceramic particles, wherein the polymer includes a structural unit derived from a first monomer, a second monomer, and a third monomer, and the molar ratio of the first monomer, the second monomer, and the third monomer is 50 to 58:40 to 44:2 to 6;
  • the first type of monomer is selected from one or more compounds of formula I:
  • R1 is selected from a hydrogen atom and a linear or branched C1-6 alkyl group
  • R2 is selected from a substituted or unsubstituted linear or branched C1-15 alkyl group, a C3-6 cycloalkyl group and an isobornyl group, and in the case of substitution, the substituent is selected from a hydroxyl group and a C1-6 chain alkyl group;
  • the second monomer is selected from one or more compounds of formula II:
  • R 3 is selected from a hydrogen atom and a linear or branched C1-6 alkyl group
  • the third monomer is selected from one or more compounds of formula III:
  • R 4 is selected from a hydrogen atom and a linear or branched C1-6 alkyl group
  • R 5 is selected from a hydrogen atom, a hydroxy C1-6 alkyl group and a C1-6 alkoxy group.
  • the adhesive composition of the present application has good bonding effect, and can increase the porosity of the isolation membrane, improve the ion conductivity, reduce the internal resistance of the isolation membrane, and enhance the cycle performance of the secondary battery.
  • the first type of monomer is an acrylate monomer, which can improve the anti-swelling ability of the binder, and as a flexible monomer segment in the molecular segment, it can adjust the glass transition temperature of the polymer, thereby helping the binder composition to play a good bonding effect.
  • the second type of monomer is an acrylonitrile monomer, which has a strong polar cyano group and helps to improve ionic conductivity.
  • the third type of monomer is an acrylamide monomer, in which the amide group mainly plays a cross-linking role and helps to adjust the molecular weight of the polymer.
  • the molar ratio of the above three types of monomers should be controlled within a certain range so that the polymer has an ideal molecular weight and glass transition temperature, thereby helping to improve ionic conductivity while ensuring the bonding performance of the binder.
  • R1 is selected from hydrogen atom and methyl
  • R2 is selected from substituted or unsubstituted straight or branched C1-6 alkyl, in the case of substitution, the substituent is hydroxyl
  • R3 is selected from hydrogen atom and methyl
  • R4 is selected from hydrogen atom and methyl
  • R5 is selected from hydrogen atom, hydroxy C1-4 alkyl and C1-4 alkoxy.
  • the first monomer is selected from methyl acrylate, ethyl acrylate, n-butyl acrylate, isobutyl acrylate, sec-butyl acrylate, tert-butyl acrylate, n-propyl acrylate, cyclohexyl acrylate, lauryl acrylate, 2-ethylhexyl acrylate, 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, methyl methacrylate, ethyl methacrylate, n-butyl methacrylate, 2-ethylhexyl methacrylate, isobornyl methacrylate, lauryl methacrylate, 2-hydroxyethyl methacrylate, and one or more of 2-hydroxypropyl methacrylate.
  • the second monomer is acrylonitrile or methacrylonitrile.
  • the third monomer is selected from one or more of acrylamide,
  • first, second and/or third monomers respectively helps to improve the ionic conductivity of the isolation membrane and increase the cycle capacity retention rate of the battery.
  • the molar ratio of the first monomer, the second monomer, and the third monomer is 50 to 57: 41 to 44: 2 to 6.
  • the molar ratio within the above range is more helpful for the binder composition to further improve the ionic conductivity of the separator and improve the cycle capacity retention rate of the battery.
  • the molar percentage of the first monomer is 50-58mol%, optionally 50-57mol%; alternatively, the molar percentage of the first monomer is 50mol%, 51mol%, 52mol%, 53mol%, 54mol%, 55mol%, 56mol%, 57mol% or 58mol%, or in the range of any two of the above values.
  • the molar percentage of the second monomer is 40-44mol%, optionally 41-44mol%; alternatively, the molar percentage of the second monomer is 40mol%, 41mol%, 42mol%, 43mol% or 44mol%, or in the range of any two of the above values.
  • the molar percentage of the third monomer is 2-6 mol%; optionally, the molar percentage of the third monomer is 2 mol%, 3 mol%, 4 mol%, 5 mol% or 6 mol%, or within the range of any two of the above values.
  • the weight ratio of the polymer to the ceramic particles is 40 to 90: 10 to 60, and optionally 50 to 80: 20 to 50.
  • the weight ratio of the polymer to the ceramic particles is within the above range, the bonding effect of the binder with the isolation membrane and the electrode can be further ensured, and the isolation membrane can have appropriate porosity and good ionic conductivity.
  • the weight average molecular weight of the polymer is 60,000 to 120,000, optionally 63,300 to 118,800.
  • the weight average molecular weight of the polymer is within the above range, so that the binder composition of the present application can have appropriate fluidity during bonding, thereby achieving a good bonding effect, thereby improving the cycle performance of the secondary battery.
  • the average particle size Dv50 of the ceramic particles is 40nm to 110nm, optionally 45nm to 106nm; alternatively, the average particle size Dv50 of the ceramic particles is 40nm, 45nm, 50nm, 56nm, 70nm, 89nm, 100nm, 106nm or 110nm, or within the range of any two of these values.
  • the average particle size Dv50 of the ceramic particles is 50nm to 100nm, more optionally 56nm to 89nm. Further controlling the average particle size of the ceramic particles can further improve the ionic conductivity and capacity retention rate.
  • the material of the ceramic particles can be any suitable conventional material in the art.
  • the ceramic particles are selected from alumina, boehmite, titanium dioxide and silicon dioxide.
  • the ceramic particles may be porous particles or solid particles (ie, non-porous particles). In some embodiments, the ceramic particles are porous particles.
  • the average pore size of the porous particles is 0.3nm to 6.0nm; alternatively, the average pore size is 0.5nm, 1nm, 1.3nm, 3nm, 3.8nm, 5nm or 5.7nm, or within a range consisting of any two of these values.
  • the average pore size is 0.5nm to 5.7nm, more optionally 1.0nm to 5.0nm, and more optionally 1.3nm to 3.8nm. Further selecting a porous particle material, and preferably controlling its average pore size, is conducive to further improving the porosity and ionic conductivity of the isolation membrane while ensuring the thermal stability of the isolation membrane, as well as the cycle capacity retention rate of the secondary battery.
  • the ceramic particles are porous silica particles.
  • the porous silica particles can further improve the porosity and ion conductivity of the separator, reduce the internal resistance of the separator, and improve the cycle performance of the secondary battery.
  • the polymer is coated on the ceramic particles. Before application, the polymer is coated on the ceramic particles to reduce or avoid the particles falling into the pores of the isolation membrane to cause pore blockage, while ensuring that the polymer and ceramic particles can be evenly applied to the substrate in an ideal ratio to achieve improved heat resistance, porosity and good bonding effect. In some embodiments, the polymer is coated on the porous silica particles.
  • the present application provides an isolation film, which includes a base layer and a coating layer disposed on at least one surface of the base layer, wherein the coating layer contains the adhesive of the present application.
  • the present application has no particular restriction on the type of material of the isolation membrane base layer, and any known porous structure base layer with good chemical stability and mechanical stability can be selected.
  • the material of the base layer of the isolation membrane can be selected from at least one of glass fiber, non-woven fabric, polyethylene, polypropylene and polyvinylidene fluoride.
  • the isolation membrane can be a single-layer film or a multi-layer composite film, without particular limitation. When the isolation membrane is a multi-layer composite film, the materials of each layer can be the same or different, without particular limitation.
  • a third aspect of the present application provides a secondary battery, comprising the binder of the present application and/or the isolation film of the present application.
  • a fourth aspect of the present application provides a battery module, comprising the secondary battery of the third aspect.
  • a fifth aspect of the present application provides a battery pack, comprising the battery module of the fourth aspect.
  • a sixth aspect of the present application provides an electrical device comprising at least one selected from the secondary battery of the third aspect, the battery module of the fourth aspect, and the battery pack of the fifth aspect.
  • a secondary battery is provided.
  • the secondary battery is a lithium ion secondary battery.
  • a secondary battery includes a positive electrode sheet, a negative electrode sheet, an electrolyte and a separator.
  • active ions are embedded and released back and forth between the positive electrode sheet and the negative electrode sheet.
  • the electrolyte plays the role of conducting ions between the positive electrode sheet and the negative electrode sheet.
  • the separator is set between the positive electrode sheet and the negative electrode sheet, mainly to prevent the positive and negative electrodes from short-circuiting, while allowing ions to pass through.
  • the positive electrode plate includes a positive electrode current collector and a positive electrode film layer arranged on at least one surface of the positive electrode current collector, wherein the positive electrode film layer includes the positive electrode active material of the first aspect of the present application.
  • the positive electrode current collector has two surfaces opposite to each other in its thickness direction, and the positive electrode film layer is disposed on any one or both of the two opposite surfaces of the positive electrode current collector.
  • the positive electrode current collector may be a metal foil or a composite current collector.
  • aluminum foil may be used as the metal foil.
  • the composite current collector may include a polymer material base and a metal layer formed on at least one surface of the polymer material base.
  • the composite current collector may be formed by forming a metal material (aluminum, aluminum alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy, etc.) on a polymer material substrate (such as a substrate of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • PP polypropylene
  • PET polyethylene terephthalate
  • PBT polybutylene terephthalate
  • PS polystyrene
  • PE polyethylene
  • the positive electrode active material may be a positive electrode active material for a battery known in the art.
  • the positive electrode active material may include at least one of the following materials: lithium-containing phosphates with an olivine structure, lithium transition metal oxides and their respective modified compounds, sodium transition metal oxides, polyanionic compounds, and Prussian blue compounds.
  • the present application is not limited to these materials, and other traditional materials that can be used as positive electrode active materials for batteries may also be used. These positive electrode active materials may be used alone or in combination of two or more.
  • lithium transition metal oxides may include, but are not limited to , lithium cobalt oxide (such as LiCoO2 ), lithium nickel oxide (such as LiNiO2 ), lithium manganese oxide (such as LiMnO2 , LiMn2O4 ), lithium nickel cobalt oxide, lithium manganese cobalt oxide, lithium nickel manganese oxide, lithium nickel cobalt manganese oxide (such as LiNi1 / 3Co1 / 3Mn1 / 3O2 (also referred to as NCM333 ), LiNi0.5Co0.2Mn0.3O2 (also referred to as NCM523 ) , LiNi0.5Co0.25Mn0.25O2 (also referred to as NCM211 ) , LiNi0.6Co0.2Mn0.2O2 (also referred to as NCM622 ), LiNi0.8Co0.1Mn0.1O2 (also referred to as NCM811 ), lithium nickel cobalt aluminum oxide (such as LiNi 0.85 Co 0.15 Al 0.05
  • lithium-containing phosphates with an olivine structure may include, but are not limited to, at least one of lithium iron phosphate (such as LiFePO 4 (also referred to as LFP)), a composite material of lithium iron phosphate and carbon, lithium manganese phosphate (such as LiMnPO 4 ), a composite material of lithium manganese phosphate and carbon, lithium iron manganese phosphate, and a composite material of lithium iron manganese phosphate and carbon.
  • lithium iron phosphate such as LiFePO 4 (also referred to as LFP)
  • LiMnPO 4 lithium manganese phosphate
  • LiMnPO 4 lithium manganese phosphate
  • LiMnPO 4 lithium manganese phosphate and carbon
  • the transition metal in the sodium transition metal oxide, may be at least one of Mn, Fe, Ni, Co, Cr, Cu, Ti, Zn, V, Zr and Ce.
  • the sodium transition metal oxide is, for example, Na x M y O 2 , wherein M is one or more of Ti, V, Mn, Co, Ni, Fe, Cr and Cu, 0 ⁇ x ⁇ 1, 0.5 ⁇ y ⁇ 1.5.
  • the positive electrode active material may be Na 0.88 Cu 0.24 Fe 0.29 Mn 0.47 O 2 .
  • the polyanionic compound may be a compound having sodium ions, transition metal ions and tetrahedral (YO 4 ) n- anion units.
  • the transition metal may be at least one of Mn, Fe, Ni, Co, Cr, Cu, Ti, Zn, V, Zr and Ce;
  • Y may be at least one of P, S and Si; and
  • n represents the valence state of (YO 4 ) n- .
  • the polyanionic compound may also be a compound having sodium ions, transition metal ions, tetrahedral (YO 4 ) n- anion units and halogen anions.
  • the transition metal may be at least one of Mn, Fe, Ni, Co, Cr, Cu, Ti, Zn, V, Zr and Ce;
  • Y may be at least one of P, S and Si, and n represents the valence state of (YO 4 ) n- ;
  • the halogen may be at least one of F, Cl and Br.
  • the polyanionic compound may also be a compound having sodium ions, tetrahedral (YO 4 ) n- anion units, polyhedral units (ZO y ) m+ and optional halogen anions.
  • Y may be at least one of P, S and Si
  • n represents the valence state of (YO 4 ) n-
  • Z represents a transition metal, which may be at least one of Mn, Fe, Ni, Co, Cr, Cu, Ti, Zn, V, Zr and Ce
  • m represents the valence state of (ZO y ) m+
  • the halogen may be at least one of F, Cl and Br.
  • the polyanionic compound is at least one of NaFePO 4 , Na 3 V 2 (PO 4 ) 3 , NaM′PO 4 F (M′ is one or more of V, Fe, Mn and Ni), and Na 3 (VO y ) 2 (PO 4 ) 2 F 3-2y (0 ⁇ y ⁇ 1).
  • the Prussian blue compound may be a compound having sodium ions, transition metal ions and cyanide ions (CN - ).
  • the transition metal may be at least one of Mn, Fe, Ni, Co, Cr, Cu, Ti, Zn, V, Zr and Ce.
  • the Prussian blue compound is, for example, Na a Me b Me' c (CN) 6 , wherein Me and Me' are each independently at least one of Ni, Cu, Fe, Mn, Co and Zn, 0 ⁇ a ⁇ 2, 0 ⁇ b ⁇ 1, 0 ⁇ c ⁇ 1.
  • the positive electrode film layer may also optionally include a binder.
  • the binder may include at least one of polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), vinylidene fluoride-tetrafluoroethylene-propylene terpolymer, vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer, tetrafluoroethylene-hexafluoropropylene copolymer, and fluorine-containing acrylate resin.
  • PVDF polyvinylidene fluoride
  • PTFE polytetrafluoroethylene
  • PTFE polytetrafluoroethylene
  • vinylidene fluoride-tetrafluoroethylene-propylene terpolymer vinylidene fluoride-hexafluoropropylene-tetrafluoroethylene terpolymer
  • the positive electrode film layer may further include a conductive agent, which may include, for example, at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • a conductive agent which may include, for example, at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene, and carbon nanofibers.
  • the positive electrode sheet can be prepared in the following manner: the components for preparing the positive electrode sheet, such as the positive electrode active material, the conductive agent, the binder and any other components are dispersed in a solvent (such as N-methylpyrrolidone) to form a positive electrode slurry; the positive electrode slurry is coated on the positive electrode collector, and after drying, cold pressing and other processes, the positive electrode sheet can be obtained.
  • a solvent such as N-methylpyrrolidone
  • the negative electrode sheet includes a negative electrode current collector and a negative electrode film layer disposed on at least one surface of the negative electrode current collector, wherein the negative electrode film layer includes a negative electrode active material.
  • the negative electrode current collector has two surfaces opposite to each other in its thickness direction, and the negative electrode film layer is disposed on any one or both of the two opposite surfaces of the negative electrode current collector.
  • the negative electrode current collector may be a metal foil or a composite current collector.
  • a metal foil a copper foil may be used.
  • the composite current collector may include a polymer material base layer and a metal layer formed on at least one surface of the polymer material substrate.
  • the composite current collector may be formed by forming a metal material (copper, copper alloy, nickel, nickel alloy, titanium, titanium alloy, silver and silver alloy, etc.) on a polymer material substrate (such as a substrate of polypropylene (PP), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polystyrene (PS), polyethylene (PE), etc.).
  • PP polypropylene
  • PET polyethylene terephthalate
  • PBT polybutylene terephthalate
  • PS polystyrene
  • PE polyethylene
  • the negative electrode active material may adopt the negative electrode active material for the battery known in the art.
  • the negative electrode active material may include at least one of the following materials: artificial graphite, natural graphite, soft carbon, hard carbon, silicon-based materials, tin-based materials, lithium titanate, etc.
  • the silicon-based material may be selected from at least one of elemental silicon, silicon oxide compounds, silicon-carbon composites, silicon-nitrogen composites, and silicon alloys.
  • the tin-based material may be selected from at least one of elemental tin, tin oxide compounds, and tin alloys.
  • the present application is not limited to these materials, and other traditional materials that can be used as negative electrode active materials for batteries may also be used. These negative electrode active materials may be used alone or in combination of two or more.
  • the negative electrode film layer may further include a binder.
  • the binder may be selected from at least one of styrene-butadiene rubber (SBR), polyacrylic acid (PAA), sodium polyacrylate (PAAS), polyacrylamide (PAM), polyvinyl alcohol (PVA), sodium alginate (SA), polymethacrylic acid (PMAA) and carboxymethyl chitosan (CMCS).
  • the negative electrode film layer may further include a conductive agent, which may be selected from at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
  • a conductive agent which may be selected from at least one of superconducting carbon, acetylene black, carbon black, Ketjen black, carbon dots, carbon nanotubes, graphene and carbon nanofibers.
  • the negative electrode film layer may optionally include other additives, such as a thickener (eg, sodium carboxymethyl cellulose (CMC-Na)).
  • a thickener eg, sodium carboxymethyl cellulose (CMC-Na)
  • the negative electrode sheet can be prepared in the following manner: the components for preparing the negative electrode sheet, such as the negative electrode active material, the conductive agent, the binder and any other components are dispersed in a solvent (such as deionized water) to form a negative electrode slurry; the negative electrode slurry is coated on the negative electrode collector, and after drying, cold pressing and other processes, the negative electrode sheet can be obtained.
  • a solvent such as deionized water
  • the electrolyte plays the role of conducting ions between the positive electrode and the negative electrode.
  • the present application has no specific restrictions on the type of electrolyte, which can be selected according to needs.
  • the electrolyte can be liquid, gel or all-solid.
  • the electrolyte is an electrolyte solution, which includes an electrolyte salt and a solvent.
  • the electrolyte salt may be selected from one or more of lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium hexafluoroarsenate, lithium bisfluorosulfonyl imide, lithium bistrifluoromethanesulfonyl imide, lithium trifluoromethanesulfonate, lithium difluorophosphate, lithium difluorooxalate borate, lithium dioxalate borate, lithium difluorodioxalate phosphate and lithium tetrafluorooxalate phosphate, sodium hexafluorophosphate (NaPF 6 ), sodium hexafluoroborate (NaBF 4 ), NaN(SO 2 F) 2 (abbreviated as NaFSI), NaClO 4 , NaAsF 6 , NaB(C 2 O 4 ) 2 (abbreviated as NaBOB), NaBF 2 (C 2 O 4 )
  • the solvent can be selected from at least one of ethylene carbonate, propylene carbonate, ethyl methyl carbonate, diethyl carbonate, dimethyl carbonate, dipropyl carbonate, methyl propyl carbonate, ethyl propyl carbonate, butylene carbonate, fluoroethylene carbonate, methyl formate, methyl acetate, ethyl acetate, propyl acetate, methyl propionate, ethyl propionate, propyl propionate, methyl butyrate, ethyl butyrate, 1,4-butyrolactone, cyclopentane sulfone, dimethyl sulfone, methyl ethyl sulfone and diethyl sulfone.
  • the electrolyte may further include additives, such as negative electrode film-forming additives, positive electrode film-forming additives, and additives that can improve certain battery properties, such as additives that improve battery overcharge performance, additives that improve battery high or low temperature performance, etc.
  • additives such as negative electrode film-forming additives, positive electrode film-forming additives, and additives that can improve certain battery properties, such as additives that improve battery overcharge performance, additives that improve battery high or low temperature performance, etc.
  • the positive electrode sheet, the negative electrode sheet, and the separator may be formed into an electrode assembly by a winding process or a lamination process.
  • the secondary battery may include an outer package for packaging the positive electrode sheet, the negative electrode sheet and the electrolyte.
  • the positive electrode sheet, the negative electrode sheet and the separator may be laminated or wound to form a laminated structure battery cell or a wound structure battery cell, and the battery cell is packaged in the outer package; the electrolyte adopts the electrolyte described in the first aspect of the present application, and the electrolyte is infiltrated in the battery cell.
  • the number of batteries in the secondary battery may be one or more, which can be adjusted according to demand.
  • the present application provides an electrode assembly.
  • the positive electrode sheet, the negative electrode sheet and the separator can be made into an electrode assembly by a winding process or a lamination process.
  • the outer packaging can be used to encapsulate the above-mentioned electrode assembly and electrolyte.
  • the outer packaging of the secondary battery may be a soft package, such as a bag-type soft package.
  • the material of the soft package may be plastic, such as one or more of polypropylene (PP), polybutylene terephthalate (PBT), polybutylene succinate (PBS), etc.
  • the outer packaging of the secondary battery may be a hard shell, such as a hard plastic shell, an aluminum shell, a steel shell, etc.
  • FIG1 is a secondary battery 5 of a square structure as an example.
  • the outer package may include a shell 51 and a cover plate 53.
  • the shell 51 may include a bottom plate and a side plate connected to the bottom plate, and the bottom plate and the side plate enclose a receiving cavity.
  • the shell 51 has an opening connected to the receiving cavity, and the cover plate 53 can be covered on the opening to close the receiving cavity.
  • the positive electrode sheet, the negative electrode sheet and the isolation film can form an electrode assembly 52 through a winding process or a lamination process.
  • the electrode assembly 52 is encapsulated in the receiving cavity.
  • the electrolyte is infiltrated in the electrode assembly 52.
  • the number of electrode assemblies 52 contained in the secondary battery 5 can be one or more, and those skilled in the art can select according to specific actual needs.
  • secondary batteries may be assembled into a battery module.
  • the number of secondary batteries contained in the battery module may be one or more, and the specific number may be selected by those skilled in the art according to the application and capacity of the battery module.
  • FIG3 is a battery module 4 as an example.
  • a plurality of secondary batteries 5 may be arranged in sequence along the length direction of the battery module 4. Of course, they may also be arranged in any other manner. Further, the plurality of secondary batteries 5 may be fixed by fasteners.
  • the battery module 4 may further include a housing having a housing space, and the plurality of secondary batteries 5 are housed in the housing space.
  • the battery modules described above may also be assembled into a battery pack.
  • the battery pack may contain one or more battery modules, and the specific number may be selected by those skilled in the art according to the application and capacity of the battery pack.
  • FIG4 and FIG5 are battery packs 1 as an example.
  • the battery pack 1 may include a battery box and a plurality of battery modules 4 disposed in the battery box.
  • the battery box includes an upper box body 2 and a lower box body 3, and the upper box body 2 can be covered on the lower box body 3 to form a closed space for accommodating the battery modules 4.
  • the plurality of battery modules 4 can be arranged in the battery box in any manner.
  • the present application also provides an electrical device, which includes at least one of the secondary battery, battery module, or battery pack provided in the present application.
  • the secondary battery, battery module, or battery pack can be used as a power source for the electrical device, and can also be used as an energy storage unit for the electrical device.
  • the electrical device may include mobile devices (such as mobile phones, laptops, etc.), electric vehicles (such as pure electric vehicles, hybrid electric vehicles, plug-in hybrid electric vehicles, electric bicycles, electric scooters, electric golf carts, electric trucks, etc.), electric trains, ships and satellites, energy storage systems, etc., but are not limited to these.
  • a secondary battery, a battery module or a battery pack may be selected according to its usage requirements.
  • Fig. 6 is an example of an electric device.
  • the electric device is a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc.
  • a battery pack or a battery module may be used.
  • a device may be a mobile phone, a tablet computer, a notebook computer, etc. Such a device is usually required to be thin and light, and a secondary battery may be used as a power source.
  • Preparation Examples 2 to 5 are the same as those of Preparation Example 1, except that the molar ratios of the three monomers are 51:43:6, 52:42:6, 53:41:6 and 54:40:6, respectively, and the total mass of the three monomers is 100 g, to prepare polymers 2 to 5.
  • the molar ratios of the three monomers are 54:43:3, 55:42:3, 56:41:3, and 57:40:3, respectively, and the total mass of the three monomers is 100 g.
  • the remaining preparation steps are the same as those in Preparation Example 1 to obtain polymers 17 to 20.
  • the molar ratios of the three monomers are 55:43:2, 56:42:2, 57:41:2, and 58:40:2, respectively, and the total mass of the three monomers is 100 g.
  • the remaining preparation steps are the same as those in Preparation Example 1 to obtain polymers 22 to 25.
  • the weight average molecular weight of polymer 1-27 and comparative polymer 1-2 obtained in the above preparation examples and comparative preparation examples was determined by using a Waters 1515 gel permeation chromatograph; wherein the mobile phase was N,N-dimethylformamide, the standard sample was a linear polymethyl methacrylate polymer with a narrow molecular weight distribution, and the solvent flow rate was 1.0 ml/min.
  • Table 1 shows the monomers and their molar ratios in the above Preparation Examples 1-27 and Comparative Preparation Examples 1-2, as well as the weight average molecular weight of the finally obtained polymers.
  • the ceramic particles in the following examples are all commercially available.
  • the average particle size Dv50 of the ceramic particles is measured by a laser particle size analyzer (using deionized water as a dispersant); the average pore size of the ceramic particles is measured by a gas adsorption-desorption isotherm method.
  • the average particle size and average pore size are shown in Table 2 below.
  • a commercially available PP-PE copolymer microporous film with a thickness of 20 ⁇ m and an average pore size of 80 nm was used as the substrate.
  • the adhesive composition prepared as described above was stirred and mixed in N-methylpyrrolidone (NMP) to obtain a slurry (solid content of 20%).
  • NMP N-methylpyrrolidone
  • the slurry was evenly coated on both surfaces of the substrate, and dried to remove the organic solvent.
  • the coating density of the adhesive composition on the substrate was 0.5 g/m 2 to obtain a separator.
  • PVDF Polyvinylidene fluoride
  • LFP lithium iron phosphate
  • NMP N-methylpyrrolidone
  • ethylene carbonate (EC), ethyl methyl carbonate (EMC), and diethyl carbonate (DEC) are mixed in a volume ratio of 1:1:1 to obtain a mixed solvent, and then LiPF6 is dissolved in the above mixed solvent to obtain an electrolyte, wherein the concentration of LiPF6 is 1 mol/L.
  • the positive electrode sheet, separator, and negative electrode sheet are stacked and wound in order, and pre-pressed (during this process, the separator and the electrode sheet are bonded) to obtain an electrode assembly; the electrode assembly is placed in an outer package, and the above-prepared electrolyte is added. After packaging, standing, formation, aging and other processes, a secondary battery is obtained.
  • Example 6 Except that the average particle diameters of the porous silica particles are changed to 45 nm, 50 nm, 56 nm, 89 nm, 100 nm and 106 nm, respectively, the other steps of Examples 6 to 11 are the same as those of Example 1.
  • Example 12 to 17 are the same as those of Example 2 except that the average pore diameters of the porous silica particles are changed to 0.5 nm, 1 nm, 1.3 nm, 3.8 nm, 5 nm and 5.7 nm, respectively.
  • Comparative Example 5 Except that the polymer is changed from Preparation Example 1 to Comparative Preparation Example C1, and the particles are changed from porous particles to solid (non-porous) particles with the same average particle size, the remaining steps of Comparative Example 5 are the same as those of Example 1.
  • Rb is the bulk resistance of the diaphragm
  • L and S are the thickness and area of the isolation diaphragm to be tested respectively.
  • Example 1 the battery capacity retention rate test process is as follows: at 25°C, the battery prepared in Example 1 is charged to 4.3V at a constant current of 1/3C, then charged to a current of 0.05C at a constant voltage of 4.3V, left for 5 minutes, and then discharged to 2.8V at 1/3C. The obtained discharge capacity is recorded as the initial capacity C 0 . The above steps are repeated for the same battery, and the discharge capacity C n of the battery after the nth cycle is recorded at the same time.
  • the battery capacity retention rate under a specific number of cycles can be used to reflect the difference in cycle performance.
  • the battery capacity retention rate data corresponding to Example 1 in Table 2 is the data measured after 100 cycles under the above test conditions.
  • the test process of the comparative example and other examples is the same as above.
  • the binder composition of the present application improves ionic conductivity and enhances the cycle performance (e.g., capacity retention rate) of the secondary battery.
  • Comparison of Examples 6 to 30 and Comparative Examples 1 to 5 shows that by controlling the content ratio of the polymer to the ceramic particles, as well as the particle size and/or average pore size of the ceramic, the obtained separator has a higher ionic conductivity and a better battery capacity retention rate.

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KR1020237038040A KR102658573B1 (ko) 2022-09-27 2022-09-27 바인더 조성물 및 이를 포함하는 분리막
EP22942941.0A EP4372049A4 (en) 2022-09-27 2022-09-27 BINDER COMPOSITION AND INSULATING FILM COMPRISING IT
JP2023568164A JP7763857B2 (ja) 2022-09-27 2022-09-27 接着剤組成物及びそれを含むセパレータ
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