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WO2024155060A1 - Composition de remplissage d'espace et bloc-batterie - Google Patents

Composition de remplissage d'espace et bloc-batterie Download PDF

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Publication number
WO2024155060A1
WO2024155060A1 PCT/KR2024/000754 KR2024000754W WO2024155060A1 WO 2024155060 A1 WO2024155060 A1 WO 2024155060A1 KR 2024000754 W KR2024000754 W KR 2024000754W WO 2024155060 A1 WO2024155060 A1 WO 2024155060A1
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WIPO (PCT)
Prior art keywords
siloxane
based resin
composition
weight
gap filler
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/KR2024/000754
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English (en)
Korean (ko)
Inventor
신우준
심민규
이동찬
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Dongwoo Fine Chem Co Ltd
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Dongwoo Fine Chem Co Ltd
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Publication of WO2024155060A1 publication Critical patent/WO2024155060A1/fr
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Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/65—Means for temperature control structurally associated with the cells
    • H01M10/655—Solid structures for heat exchange or heat conduction
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
    • C08K3/013—Fillers, pigments or reinforcing additives
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/38—Boron-containing compounds
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K9/00—Use of pretreated ingredients
    • C08K9/08—Ingredients agglomerated by treatment with a binding agent
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
    • C08L83/04—Polysiloxanes
    • 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
    • H01M10/60—Heating or cooling; Temperature control
    • H01M10/61—Types of temperature control
    • H01M10/613—Cooling or keeping cold
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/204—Racks, modules or packs for multiple batteries or multiple cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/218—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/218—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material
    • H01M50/22—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by the material of the casings or racks
    • H01M50/222—Inorganic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/233—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions
    • H01M50/24—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions adapted for protecting batteries from their environment, e.g. from corrosion
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/233—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions
    • H01M50/242—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders characterised by physical properties of casings or racks, e.g. dimensions adapted for protecting batteries against vibrations, collision impact or swelling
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/18—Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20—Oxides; Hydroxides
    • C08K3/22—Oxides; Hydroxides of metals
    • C08K2003/2227—Oxides; Hydroxides of metals of aluminium
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/38—Boron-containing compounds
    • C08K2003/382—Boron-containing compounds and nitrogen
    • C08K2003/385—Binary compounds of nitrogen with boron
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00—Specific properties of additives
    • C08K2201/002—Physical properties
    • C08K2201/005—Additives being defined by their particle size in general
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00—Polymer mixtures characterised by other features
    • C08L2205/02—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group
    • C08L2205/025—Polymer mixtures characterised by other features containing two or more polymers of the same C08L -group containing two or more polymers of the same hierarchy C08L, and differing only in parameters such as density, comonomer content, molecular weight, structure
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2205/00—Polymer mixtures characterised by other features
    • C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
    • 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 gap filler compositions and battery packs. More specifically, it relates to a gap filler composition containing a siloxane-based resin and a battery pack containing a gap filler formed using the same.
  • Secondary batteries are batteries that can be repeatedly charged and discharged, and are widely used as a power source for portable electronic devices such as mobile phones and laptop PCs.
  • lithium secondary batteries have high operating voltage, energy density, and rate characteristics, and have recently been used as a power source for electric vehicles.
  • a battery cell is defined by a lithium secondary battery, and a battery module is formed by gathering a plurality of battery cells.
  • the battery modules can be assembled to form a high-capacity/high-output battery pack applicable to electric vehicles.
  • the battery pack may be seated on a battery support plate and a gap filler composition may be used to secure the battery pack.
  • the gap filler composition application process may be included in the entire electric vehicle production platform. Therefore, in order to maintain automobile process efficiency/reliability, a gap filler composition that cures within a predetermined time and provides desired physical properties may be needed.
  • One object of the present invention is to provide a gap filler composition that provides improved curing properties and thermal properties.
  • One object of the present invention is to provide a battery pack including a gap filler formed from the gap filler composition.
  • Siloxane-based resin including first alumina particles having an average particle diameter (D50) of 5 ⁇ m or more and less than 15 ⁇ m; Second alumina particles with an average particle diameter (D50) of 15 ⁇ m to 30 ⁇ m; and third alumina particles having an average particle diameter (D50) of 60 ⁇ m to 80 ⁇ m, the content of the filler in the total weight of the composition is 80% by weight to 95% by weight, and the content of the first alumina particles in the total weight of the filler.
  • D50 average particle diameter
  • third alumina particles having an average particle diameter (D50) of 60 ⁇ m to 80 ⁇ m the content of the filler in the total weight of the composition is 80% by weight to 95% by weight, and the content of the first alumina particles in the total weight of the filler.
  • the siloxane-based resin includes a first siloxane-based resin having a vinyl end group and a second siloxane-based resin having hydrogen end groups directly bonded to silicon atoms at both ends.
  • the first siloxane-based resin is a low-viscosity siloxane-based resin having a viscosity ranging from 200 cps to 400 cps, a medium-viscosity siloxane-based resin having a viscosity ranging from 800 cps to 1,200 cps, and a viscosity ranging from 18,000 cps to 22,000 cps.
  • a gap filler composition comprising at least two types of siloxane-based resins among high-viscosity siloxane-based resins having a viscosity in the cps range.
  • the gap filler composition is manufactured as a two-part composition separated into a main composition and a cross-linking composition, the first siloxane-based resin is included in the main composition, and the second siloxane-based resin is the cross-linking composition.
  • Gap filler compositions according to exemplary embodiments of the present invention may include a plurality of types of alumina particles having different particle sizes. Therefore, the thermal conductivity of the gap filler is more effectively improved, and when applied to a vehicle battery pack, it can promote rapid heat dissipation even when the temperature increases due to repeated charging/discharging of the battery pack.
  • alumina particles of a plurality of particle size ranges can be used to more effectively lower the specific gravity of the gap filler composition while improving or maintaining thermal conductivity.
  • the gap filler composition may include multiple types of siloxane-based resins having different viscosity ranges. Therefore, the curing speed of the gap filler composition can be improved and the target hardness can be secured within a predetermined time range.
  • FIG. 1 is a schematic perspective view showing a battery pack according to example embodiments.
  • a gap filler composition comprising a siloxane-based resin, a catalyst and a filler and having improved heat conduction properties and physical properties is provided. Additionally, according to embodiments of the present invention, a battery pack using the gap filler composition is provided.
  • Gap filler compositions may include a siloxane-based resin, a catalyst, and a filler.
  • the siloxane-based resin may be provided as a base component that provides curability of the gap filler composition.
  • the siloxane-based resin may include a first siloxane-based resin and a second siloxane-based resin.
  • the first siloxane-based resin may be a siloxane-based resin containing a crosslinkable end group. According to exemplary embodiments, the first siloxane-based resin may be a siloxane-based resin containing vinyl groups at both ends of the molecule.
  • the first siloxane-based resin may include a compound represented by the following formula (1).
  • the weight average molecular weight of the first siloxane-based resin may be 10,000 to 50,000, preferably 10,000 to 30,000, and more preferably 10,000 to 25,000.
  • the first siloxane-based resin may include multiple types of resins having different viscosity ranges.
  • the first siloxane-based resin may include at least two types of resins among a low-viscosity siloxane-based resin, a medium-viscosity siloxane-based resin, and a high-viscosity siloxane-based resin whose viscosity increases sequentially.
  • the viscosity (viscosity at 25 o C) of the low viscosity siloxane-based resin may be 200 cps to 400 cps, preferably 200 cps to 300 cps, more preferably 250 cps to 300 cps. there is.
  • the viscosity (viscosity at 25 o C) of the medium viscosity siloxane-based resin may be 800 cps to 1,200 cps, preferably 900 cps to 1,100 cps, and more preferably 950 cps to 1,050 cps.
  • the viscosity (viscosity at 25 o C) of the high viscosity siloxane resin may be 18,000 cps to 22,000 cps, preferably 19,000 cps to 21,000 cps, and more preferably 19,500 cps to 20,500 cps.
  • the first siloxane-based resin includes the medium viscosity siloxane-based resin and may further include at least one of the low-viscosity siloxane-based resin and the high-viscosity siloxane-based resin.
  • the first siloxane-based resin may include the low-viscosity siloxane-based resin, the medium-viscosity siloxane-based resin, and the high-viscosity siloxane-based resin.
  • the content of the low-viscosity siloxane-based resin is 0.5% to 2% by weight
  • the content of the medium-viscosity siloxane-based resin is 70% to 90% by weight
  • the high-viscosity siloxane-based resin The content of the acid-based resin may be 10% by weight to 20% by weight.
  • the content of the low-viscosity siloxane-based resin is 0.5% by weight to 1.5% by weight
  • the content of the medium-viscosity siloxane-based resin is 80% by weight to 90% by weight
  • the high viscosity may be 10% by weight to 15% by weight.
  • the curing speed of the gap filler composition can be accelerated while maintaining the dispersibility and flowability of the resin. Therefore, the desired target hardness can be secured within a limited process time, and thermal stability can be quickly obtained.
  • the basic resin matrix and crosslinking points are formed through the medium viscosity siloxane resin, and the curing speed and mechanical strength are improved by adding low and high viscosity siloxane resins. You can do it.
  • n can be adjusted considering the molecular weight and viscosity range.
  • n may be a natural number in the range of 80 to 800, 100 to 800, 130 to 700, or 150 to 700.
  • the content of the first siloxane-based resin in the total weight of the gap filler composition may be 2% to 15% by weight, preferably 2% to 10% by weight. In the above content range, a gap filler with appropriate hardness and elasticity can be effectively formed.
  • the second siloxane-based resin may be a siloxane-based resin with a different structure from the first siloxane-based resin.
  • the second siloxane-based resin is included as a chain extender or chain regulator in the gap filler composition, and can control the overall viscosity, flowability, crosslinking properties, etc. of the composition.
  • the second siloxane-based resin may be a siloxane-based resin that does not include a crosslinkable group at the terminal.
  • both ends of the second siloxane-based resin may be hydrogen (H) capped.
  • the second siloxane-based resin may include a compound represented by Formula 2 below.
  • the weight average molecular weight of the second siloxane-based resin may be 10,000 to 50,000, preferably 10,000 to 30,000, and more preferably 10,000 to 25,000.
  • the viscosity of the second siloxane-based resin at 25 o C may be 100 cps to 1,500 cps, preferably 200 cps to 1,500 cps, and more preferably 300 cps to 1,200 cps.
  • the curing properties and curing speed described later can be more easily secured, and appropriate application characteristics and flowability of the gap filler composition can be secured.
  • m can be adjusted considering the molecular weight and viscosity range.
  • m may be a natural number in the range of 20 to 700, 30 to 700, 50 to 700, 100 to 700, or 130 to 700.
  • the content of the second siloxane-based resin in the total weight of the gap filler composition may be 2% to 15% by weight, preferably 2% to 10% by weight. In the above content range, a gap filler with appropriate hardness and elasticity can be effectively formed.
  • the catalyst may be used as a regulator to obtain curing properties and curing speed, which will be described later, by promoting crosslinking and/or interaction between the first siloxane-based resin and/or the second siloxane-based resin of the gap filler composition.
  • the catalyst may include an organic-inorganic hybrid catalyst containing platinum and silicon.
  • the catalyst may contain Pt atoms and Si 2 O groups (-Si-O-Si-) in the molecule.
  • silicon (Si) atoms of the Si 2 O group are bonded to vinyl groups, and Pt atoms can be coordinated or captured by the vinyl groups.
  • the content of the catalyst based on the total weight of the composition may be 0.02% by weight to 0.05% by weight. Within the above range, an appropriate curing speed can be achieved while preventing excessive hardness/elasticity increase of the gap filler.
  • the filler may be included as a component that improves the heat dissipation characteristics of the battery pack by increasing the thermal conductivity of the gap filler.
  • the filler is alumina (Al 2 O 3 ), aluminum nitride (AlN), boron nitride (BN), silicon nitride, SiC, ZnO, aluminum hydroxide (Al(OH) 3 ), boehmite, BeO, etc. may be included.
  • the filler may include alumina.
  • the filler may include alumina surface-treated with a silane agent.
  • the silane agent can be chemically bonded or attached to the surface of the alumina particle and stabilize the filler through interaction with the siloxane-based resin described above.
  • the filler can be uniformly dispersed in the gap filler composition, thereby realizing uniform heat conduction characteristics within the battery pack.
  • the silane agent may include three alkoxy groups and one alkyl group directly bonded to a silicon atom.
  • the alkoxy group may be a methoxy group.
  • the carbon number of the alkyl group included in the silane agent may be 8 or more. In this case, interaction with the siloxane-based resin can be effectively promoted.
  • the alkyl group included in the silane agent may have 8 to 16 carbon atoms, preferably 8 to 12 carbon atoms. In this case, it is possible to prevent a decrease in dispersibility due to an excessive increase in the number of carbon atoms.
  • the filler may include multiple types of alumina particles having different average particle diameters. Accordingly, the packing and distribution characteristics of the alumina particles in the composition can be improved, and the heat conduction characteristics can be improved.
  • the alumina particles may include first alumina particles, second alumina particles, and third alumina particles whose average particle diameters sequentially increase.
  • the average particle diameter (D50) of the first alumina particles may be less than 15 ⁇ m.
  • the average particle diameter (D50) of the second alumina particles may be 15 ⁇ m to 30 ⁇ m.
  • the average particle diameter (D50) of the third alumina particles may be 50 ⁇ m or more.
  • the average particle diameter (D50) of the first alumina particles may be 5 ⁇ m to 13 ⁇ m.
  • the average particle diameter (D50) of the second alumina particles may be 15 ⁇ m to 25 ⁇ m.
  • the average particle diameter (D50) of the third alumina particles may be 60 ⁇ m to 80 ⁇ m.
  • average particle diameter (D50) used in this application may refer to the median particle diameter corresponding to 50% of the cumulative distribution (based on number) in which the particles are arranged in size order.
  • the filler may be included in the largest amount of the gap filler composition.
  • the filler may be included in the remaining amount excluding the above-described siloxane-based resin and the catalyst in the gap filler composition.
  • the term “remaining amount” used in this application is used as a variable amount that changes depending on the amount of the additive when the gap filler composition includes additives other than the siloxane-based resin, the catalyst, and the filler.
  • the remaining amount may be the amount excluding the siloxane-based resin, the catalyst, and the additive from the total weight of the composition.
  • the content of the filler may be 80% to 95% by weight of the total weight of the composition (eg, solid content). If the content of the filler is less than 80 weight, sufficient thermal conductivity of the gap filler may not be secured. If the content of the filler exceeds 95% by weight, the specific gravity of the gap filler composition and the gap filler may excessively increase, and the brittleness of the gap filler may increase.
  • the content of the filler may be 85% by weight to 95% by weight, more preferably 87% by weight to 91% by weight.
  • the amount of the filler is calculated to include the amount of the surface-treated silane agent.
  • tertiary alumina particles may be included in the largest amount among the fillers. Accordingly, the heat conduction efficiency through the filler can be sufficiently increased.
  • the content of the third alumina particles is 50% by weight to 70% by weight
  • the content of the second alumina particles is 10% by weight to 30% by weight
  • the content of the first alumina particles is 10% by weight. It may be from 30% by weight.
  • the content of the third alumina particles provided as large-diameter particles is 55% to 65% by weight
  • the content of the second alumina particles is 15% to 25% by weight
  • the first alumina particles Their content may be 15% by weight to 25% by weight.
  • the second alumina particles and the first alumina particles which are provided as medium-diameter particles and small-diameter particles, are distributed together in similar or equal amounts, preventing an increase in the brittleness of the gap filler due to the filler and maintaining heat conduction properties. can be maintained.
  • the gap filler composition may further include additives to improve conductivity and curability of the composition within a range that does not inhibit the actions of the above-described siloxane-based resin, the catalyst, and the filler.
  • the additives may include flame retardants, surfactants, silane coupling agents, colorants, antioxidants, plasticizers, etc.
  • examples of the flame retardant include organic flame retardants such as melamine cyanurate, and inorganic flame retardants such as magnesium hydroxide.
  • a liquid type flame retardant material such as triethyl phosphate (TEP) or tris(1,3-chloro-2-propyl)phosphate (TCPP) may be used.
  • examples of the surfactant include polyethylene glycol, polypropylene glycol, oleic acid ethoxylate, alkylphenol ethoxylate, copolymers of ethylene oxide and propylene oxide, silicone polymers, etc.
  • silane coupling agent examples include ⁇ -glycidoxypropyltrimethoxysilane, ⁇ -glycidoxypropylmethyldiethoxysilane, ⁇ -glycidoxypropyltriethoxysilane, 3-mercaptopropyltrimethoxysilane, Vinyltrimethoxysilane, vinyltriethoxysilane, ⁇ -methacryloxypropyltrimethoxysilane, ⁇ -methacryloxypropyltriethoxysilane, ⁇ -aminopropyltrimethoxysilane, ⁇ -aminopropyltriethoxy Silane, 3-isocyanate propyltriethoxysilane, ⁇ -acetoacetate propyltrimethoxysilane, etc. are mentioned.
  • antioxidant phenol-based compounds, quinone-based compounds, amine-based compounds, phosphorus-based compounds, phosphite-based compounds, thioether-based compounds, etc. may be used.
  • plasticizer tetraethylene glycol monobutyl ether (3,6,9,12-tetraoxahexadecanol), triethylene glycol monobutyl ether (3,6,9-trioxatridecanol), diethylene glycol monobutyl Ether (2-(2-butoxyethoxy)ethanol), propylene glycol monobutyl ether, ethylene glycol monobutyl ether, propylene glycol monomethyl ether (1-methoxy-2-propanol), propylene glycol monomethyl ether acetate, Polyethylene glycol, glycerin, etc. can be mentioned.
  • the gap filler composition may be prepared as a two-component composition.
  • the gap filler composition may be prepared by separately preparing the main composition and the cross-linking composition and then mixing the main composition and the cross-linking composition.
  • the main composition may include the first siloxane-based resin, the catalyst, and the filler.
  • the crosslinking composition may include the second siloxane-based resin and the filler.
  • the second siloxane-based resin may be mixed in the main composition while the catalyst is distributed in the first siloxane-based resin. Therefore, since the second siloxane-based resin is introduced while the crosslinking points in the main composition are distributed, curing efficiency can be improved.
  • the filler may be divided and included in the main composition and the crosslinking composition.
  • the ratio of the amount of the filler contained in the main composition to the amount of the filler contained in the crosslinking composition may be 0.4 to 0.6, preferably 0.45 to 0.55. In the above ratio range, heat conduction efficiency can be improved through uniform distribution of the filler.
  • a cross-linking siloxane resin may be added to the cross-linking composition in addition to the second siloxane-based resin.
  • the cross-linked siloxane resin includes a siloxane resin of relatively low viscosity, and, like the second siloxane-based resin, may be a siloxane resin in which both ends are capped with hydrogen (H).
  • the crosslinked siloxane resin may have a viscosity of 30 cps to 120 cps, preferably 50 cps to 100 cps, and more preferably 60 cps to 90 cps.
  • the cross-linked siloxane resin may be included in an amount of 0.05% to 0.5% by weight compared to the weight of the second siloxane-based resin.
  • Shore 00 hardness measured after application of the gap filler composition and leaving it for 60 minutes at 23 o C and 50% relative humidity may be 40 to 70.
  • the process time for applying the battery pack to an electric vehicle may increase, reducing overall production efficiency. Additionally, the curability of the gap filler may be too low, which may reduce the mechanical stability of the battery pack.
  • the hardness after being left for 60 minutes may be 50 to 70, more preferably 50 to 65.
  • the Shore 00 hardness can be measured according to the ASTM D 2240 standard.
  • the Shore 00 hardness can be measured for a cured film obtained by applying the gap filler composition to a thickness of 6 mm and then curing it.
  • the specific gravity of the gap filler composition may be less than 3, preferably less than 2.5.
  • the gap filler composition may have a specific gravity of 1.9 to 2.9, preferably 2.3 to 2.7.
  • the specific gravity is a value measured relative to the standard density of water at 4 o C under 1 atmosphere.
  • the gap filler composition contains alumina particles of different particle sizes within a predetermined content range, and can achieve high thermal conductivity with a relatively low specific gravity.
  • siloxane-based resins of different viscosity ranges are included, enabling rapid curing characteristics and desired hardness/elasticity with a low specific gravity composition.
  • FIG. 1 is a schematic perspective view showing a battery pack according to example embodiments.
  • the battery pack 100 includes a battery module 110 and a support plate 130, and may include a gap filler 120 formed on the battery module 110 and the support plate 130.
  • the battery module 110 may include a plurality of battery cells 112.
  • Each of the battery cells 112 may include an electrode assembly including an anode and a cathode that are alternately and repeatedly stacked.
  • the anode and cathode may be repeatedly stacked alternately with a separator in between.
  • the positive electrode includes lithium metal oxide as a positive electrode active material, and the battery cell 112 can be provided as a lithium secondary battery.
  • the plurality of battery cells 112 each include a positive electrode lead and a negative electrode lead, and the positive electrode leads and the negative electrode leads may be merged with each other through a bus bar to define the battery module 110.
  • the battery module 110 may be fixed on the support plate 130.
  • the gap filler 120 may be formed between the battery module 110 and the support plate 130 by applying and curing the gap filler composition according to the above-described embodiments.
  • the battery module 110 can be stably fixed on the support plate 130 by the gap filler 120.
  • the gap filler 120 has stable curing properties and may have improved heat conduction properties.
  • the gap filler composition has a low specific gravity and can maintain the target hardness range over a predetermined time range. Therefore, stable hardness characteristics can be maintained without impairing the overall electric vehicle process efficiency or increasing the weight of the battery pack.
  • the gap filler 120 may be provided as a heat conductive layer.
  • the thermal conductivity of gap filler 120 may be about 3 W/mK.
  • the thermal conductivity of the gap filler 120 may be 10 W/mk or less.
  • the thermal conductivity of the gap filler 120 may be 3 W/mK to 5 W/mK.
  • the thermal conductivity can be measured according to the ASTM D5470 standard.
  • the filler was equally included in the main composition and the crosslinking composition in the amounts shown in Tables 1 and 2, respectively.
  • the main composition and the crosslinking composition were prepared by putting the ingredients in Tables 1 and 2, respectively, into a paste mixer, mixing and stirring for 3 minutes at 600 rpm/500 rpm rotation, and defoaming for 10 minutes at 1000 rpm/100 rpm rotation in a vacuum. It has been done.
  • Example 1 Example 2
  • Example 3 Example 4
  • Example 5 subject composition 1st siloxane type profit A-1 0.15 0.29 - 0.22 - A-2 1.72 - 0.29 2.50 - A-3 12.87 14.47 14.44 19.15 - A-4 - - - 13.28 catalyst
  • B-1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 bridge composition
  • C-2 0.015 0.015 0.015 2.140 0.015 filling D1 71.55 71.55 71.55 67.53 71.55 D2 23.85 23.85 23.85 22.51 23.85 D3 23.85 23.85 23.85 22.51 23.85
  • Comparative example 1 subject composition 1st siloxane type profit A-1 0.41 0.04 0.15 0.15 0.15 0.15 A-2 4.68 0.47 1.72 1.72 1.72 1.72 A-3 35.91 3.59 12.87 12.87 12.87 12.87 A-4 - - - - - catalyst B-1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 bridge composition 2nd siloxane type profit C-1 35.75 3.98 14.591 14.591 14.591 14.591 - C-2 4.02 0.4 0.015 0.015 0.015 0.015 - filling D-1 56.27 77.98 - 71.55 71.55 39.75 71.55 D-2 18.76 25.99 104.56 - 47.7 39.75 23.85 D-3 18.76 25.99 14.69 47.7 - 39.75 23.85 23.85
  • Second siloxane-based resin cross-linked siloxane resin (C-2): polydimethylsiloxane resin (viscosity 65 cps) with both ends hydrogenated (product name: DW520, Dami Polychem)
  • the main composition and crosslinking composition of Examples and Comparative Examples were mixed at a mass ratio of 1:1 using a two-component cartridge and cured to form a resin layer.
  • the thermal conductivity of the resin layer was measured using Hot Disk measuring equipment according to ISO22007-2 standards. Specifically, a numerical layer with a width/length of 20 mm and a thickness of 6.0 mm was formed, and the average value was calculated after measuring a total of three times.
  • a gap filler composition was prepared by mixing the main composition and crosslinking composition of Examples and Comparative Examples at a mass ratio of 1:1 using a two-component cartridge.
  • the specific gravity of the gap filler composition was measured according to Test Method A of ASTM D792.
  • the weight of the composition and the weight of the composition in water were measured according to the above standards, and then the specific gravity was calculated from the measured weight difference.
  • the main composition and cross-linking composition of the examples and comparative examples were mixed and filled at a mass ratio of 1:1 using a two-component cartridge, applied to a JIG with a thickness of 6 mm, and then heated at 23 o C and relative humidity of 50%.
  • the hardness of the cargo surface was measured according to ASTM D 2240 standard. When measuring hardness, an ASKER Durometer device was used. The hardening was performed with a load of about 0.5 kg applied, and Shore00/A hardness was evaluated by checking the stabilized measurement value 15 seconds after the load was removed every 10 minutes.
  • Hardness was measured 60 minutes after the start of curing under the above conditions.
  • Comparative example 1 Comparative example 1
  • Comparative example 2 Comparative example 3
  • Comparative example 6 Comparative example 7 thermal conductivity (W/mK) 0.7 3.3 1.8 1.9 2.1 1.8 Cross-linking reaction does not proceed importance 1.9 3.6 2.7 2.8 2.9 2.5 Hardness after 60 minutes 50 67 54 35 34 58
  • three types of alumina particles with different particle size ranges have improved thermal conductivity and low specific gravity in the examples in which the content ranges from 80% to 95% by weight, and rapid curing characteristics. provided.
  • Example 4 thermal conductivity was relatively reduced in Example 4, in which the total weight of alumina was reduced.
  • Example 5 where a single type of first siloxane resin was used, hardness was relatively reduced after 60 minutes.
  • Comparative Example 1 where the content of alumina particles was less than 80% by weight, thermal conductivity was significantly reduced, and in Comparative Example 2, where the content of alumina particles was more than 95% by weight, specific gravity increased excessively.

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Abstract

Une composition de remplissage d'espace selon des modes de réalisation de la présente invention comprend une résine à base de siloxane, un catalyseur et une charge. La charge comprend des premières particules d'alumine ayant un diamètre de particule moyen (D50) de 5 µm ou plus et moins de 15 µm, des deuxièmes particules d'alumine ayant un diamètre de particule moyen (D50) de 15 µm à 30 µm, et des troisièmes particules d'alumine ayant un diamètre de particule moyen (D50) de 60 µm à 80 µm. La teneur de la charge dans le poids total de la composition est de 80% en poids à 95% en poids, la teneur des premières particules d'alumine dans le poids total de la charge est de 15% en poids à 25% en poids, la teneur des deuxièmes particules d'alumine dans le poids total de la charge est de 15% en poids à 25% en poids, et la teneur des troisièmes particules d'alumine dans le poids total de la charge est de 55% en poids à 65% en poids. La résine à base de siloxane comprend une première résine à base de siloxane ayant des groupes terminaux vinyliques et une seconde résine à base de siloxane ayant des groupes terminaux hydrogène directement liés à des atomes de silicium aux deux extrémités.
PCT/KR2024/000754 2023-01-17 2024-01-16 Composition de remplissage d'espace et bloc-batterie Ceased WO2024155060A1 (fr)

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KR101823783B1 (ko) * 2016-10-12 2018-01-30 주식회사 케이씨씨 실리콘 고무 조성물 및 이의 경화물
KR102024524B1 (ko) * 2018-04-27 2019-10-01 주식회사 엘투와이 전기자동차 배터리 팩용 방열패키지 제조방법과 이에 의해 제조된 배터리 팩용 방열 패키지
KR102075461B1 (ko) * 2018-07-12 2020-02-10 주식회사 에이치알에스 고방열 액상 실리콘 조성물
KR102298511B1 (ko) * 2019-09-26 2021-09-07 주식회사 케이씨씨실리콘 방열 접착제 조성물
KR20220043776A (ko) * 2020-09-29 2022-04-05 주식회사 엘지에너지솔루션 수지 조성물

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KR102402503B1 (ko) 2022-02-17 2022-05-26 주식회사 서연이화 갭필러 두께 가변 적용을 통한 배터리팩 냉각구조

Patent Citations (5)

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Publication number Priority date Publication date Assignee Title
KR101823783B1 (ko) * 2016-10-12 2018-01-30 주식회사 케이씨씨 실리콘 고무 조성물 및 이의 경화물
KR102024524B1 (ko) * 2018-04-27 2019-10-01 주식회사 엘투와이 전기자동차 배터리 팩용 방열패키지 제조방법과 이에 의해 제조된 배터리 팩용 방열 패키지
KR102075461B1 (ko) * 2018-07-12 2020-02-10 주식회사 에이치알에스 고방열 액상 실리콘 조성물
KR102298511B1 (ko) * 2019-09-26 2021-09-07 주식회사 케이씨씨실리콘 방열 접착제 조성물
KR20220043776A (ko) * 2020-09-29 2022-04-05 주식회사 엘지에너지솔루션 수지 조성물

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