WO2018194171A1 - 電池用包装材料、その製造方法、及び電池 - Google Patents

電池用包装材料、その製造方法、及び電池 Download PDF

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Publication number
WO2018194171A1
WO2018194171A1 PCT/JP2018/016359 JP2018016359W WO2018194171A1 WO 2018194171 A1 WO2018194171 A1 WO 2018194171A1 JP 2018016359 W JP2018016359 W JP 2018016359W WO 2018194171 A1 WO2018194171 A1 WO 2018194171A1
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WO
WIPO (PCT)
Prior art keywords
heat
layer
packaging material
fusible resin
resin layer
Prior art date
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/JP2018/016359
Other languages
English (en)
French (fr)
Japanese (ja)
Inventor
大佑 安田
陽祐 早川
かおる 津森
山下　孝典
山下　力也
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Dai Nippon Printing Co Ltd
Original Assignee
Dai Nippon Printing Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Priority to CN201880003134.5A priority Critical patent/CN109564995B/zh
Priority to KR1020247030619A priority patent/KR20240144420A/ko
Priority to KR1020197027134A priority patent/KR102308638B1/ko
Priority to KR1020227023290A priority patent/KR20220101016A/ko
Priority to JP2018553495A priority patent/JP6465261B1/ja
Priority to KR1020217031018A priority patent/KR102419865B1/ko
Application filed by Dai Nippon Printing Co Ltd filed Critical Dai Nippon Printing Co Ltd
Priority to EP18787250.2A priority patent/EP3614449B1/en
Priority to EP24190388.9A priority patent/EP4428996A3/en
Priority to US16/604,895 priority patent/US20200194737A1/en
Publication of WO2018194171A1 publication Critical patent/WO2018194171A1/ja
Anticipated expiration legal-status Critical
Priority to US18/230,894 priority patent/US20230387519A1/en
Ceased legal-status Critical Current

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    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a packaging material for a battery, a manufacturing method thereof, and a battery.
  • recesses are formed by cold forming, and battery elements such as electrodes and electrolytes are arranged in the spaces formed by the recesses, and the heat-fusible resin layers Is heat-sealed to obtain a battery in which the battery element is accommodated in the battery packaging material.
  • the barrier layer is generally composed of an inorganic material having low moisture permeability.
  • the inorganic material and the heat-fusible resin layer are different materials, there is a problem that the adhesive strength between the barrier layer and the heat-fusible resin layer is likely to decrease. For this reason, in order to improve adhesive strength, an adhesive layer may be provided between these layers.
  • the heat-fusible resin layers are heat-sealed by applying high temperature and high pressure to the battery packaging material using a metal plate or the like.
  • the adhesive layer is crushed and the sealing strength of the battery packaging material is reduced.
  • the first aspect of the present invention is a battery packaging composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order.
  • the main object of the present invention is to provide a battery packaging material that effectively suppresses the collapse of the adhesive layer when the heat-fusible resin layers are heat-sealed, and exhibits high sealing strength in a high-temperature environment.
  • a process as shown in the schematic diagram of FIG. 10 is performed.
  • a rectangular battery packaging material 10 is formed to form a packaging body having an accommodation space (A) for accommodating a battery element such as an electrolytic solution.
  • the packaging body is folded in half, and the two edges (10a) including the edge where the terminals 15 exist are heat-sealed in a state where the terminals 15 protrude from one side of the packaging body.
  • a battery element such as an electrolytic solution is put into the housing space (A) from the opening (10b) on the outer peripheral side of the blank area 10d.
  • the opening (10b) is heat-sealed.
  • batteries for vehicles, batteries for mobile devices, and the like may be used in a high temperature environment, these batteries use an electrolyte solution having excellent heat resistance, and after storing the electrolyte solution or the like. The aging process is also performed in a high temperature environment.
  • the second aspect of the present invention provides a battery packaging material comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order. Even in the case where the electrolyte is in contact with the heat-fusible resin layer in the environment and the heat-fusible resin layers are heat-sealed with the electrolyte being adhered to the heat-fusible resin layer,
  • the main object is to provide a battery packaging material that exhibits high sealing strength.
  • a recess is formed by cold forming, and a battery element or the like is accommodated in the recess.
  • a lubricant may be used for the purpose of improving the moldability of the battery packaging material.
  • a technique of adding a lubricant to the heat-fusible resin layer located in the innermost layer is known.
  • a lubricant is added to the heat-fusible resin layer, as a mold for molding battery packaging materials, for example, it has high surface smoothness (for example, JIS B 0659-1: 2002 Annex 1 (reference) for comparison)
  • the surface Rz maximum height roughness
  • a stainless steel mold is used, the mold and the heat-fusible resin layer Therefore, the surface of the heat-fusible resin layer is easily scraped, and the lubricant located on the surface part of the heat-fusible resin layer adheres to the mold when the battery packaging material is molded.
  • the mold may become contaminated.
  • the lubricant solidified on the mold surface may be transferred to the heat-fusible resin layer of the battery packaging material. If it is subjected to heat fusion in a state in which a lump of lubricant has adhered to the heat-fusible resin layer, the melted portion of the portion to which the lubricant has adhered will become uneven, causing problems such as reduced seal strength. . In order to prevent this, it becomes necessary to increase the frequency of cleaning for removing the lubricant adhering to the mold, and there is a problem that the continuous productivity of the battery is lowered.
  • the size of the mold is large (that is, the area where the mold contacts the battery packaging material is large), and the mold is easily contaminated with a lubricant. .
  • die with a lubricant effectively is ensured, ensuring the outstanding moldability of the packaging material for batteries.
  • the third aspect of the present invention is a battery packaging material comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the main object of the present invention is to provide a battery packaging material that suppresses contamination of the mold at the time and exhibits high sealing strength by heat fusion.
  • the present inventors have intensively studied to solve the problem concerning the first aspect.
  • it is composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order, and logarithmic attenuation at 120 ° C. in the rigid pendulum measurement of the adhesive layer.
  • the battery packaging material having a rate ⁇ E of 2.0 or less effectively suppresses the crushing of the adhesive layer when the heat-fusible resin layers are heat-sealed to each other, and exhibits high sealing strength in a high-temperature environment. I found out.
  • the first aspect of the present invention has been completed by further studies based on these findings.
  • the present inventors have intensively studied to solve the problem regarding the second aspect.
  • the temperature difference T 1 and the temperature difference T are obtained by the following method. 2 is measured, the value obtained by dividing the temperature difference T 2 by the temperature difference T 1 (ratio T 2 / T 1 ) is 0.60 or more. Even when the electrolyte solution contacts the adhesive resin layer and the electrolyte solution adheres to the heat-fusible resin layer, the heat-sealing resin layers are heat-sealed with each other. I found out that it works.
  • the heat-fusible resin layer is a solution in which the concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: 1. It is made to dry after leaving still for 72 hours in electrolyte solution which is.
  • a temperature difference T 2 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer after drying is measured.
  • a solution having a 1: 1: 1 volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is obtained by mixing ethylene carbonate, diethyl carbonate, and dimethyl carbonate in a volume ratio of 1: 1: 1. The resulting solution.
  • FIG. 11 schematically shows the temperature difference T 1 and the temperature difference T 2 in the differential scanning calorimetry.
  • the start point (extrapolation melting start temperature) is indicated by Ts
  • the end point (extrapolation melting end temperature) is indicated by Te.
  • the temperature difference T 2 is smaller than the temperature difference T 1 .
  • the second aspect of the present invention has been completed by further studies based on these findings.
  • the present inventors have intensively studied to solve the problem concerning the third aspect.
  • it is composed of a laminate comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order, and the heat-fusible resin layer contains a lubricant, and is JIS K7161.
  • the third aspect of the present invention has been completed by further studies based on these findings.
  • Item 1 It is composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order,
  • the adhesive layer is a battery packaging material whose logarithmic decay rate ⁇ E at 120 ° C. in a rigid pendulum measurement is 2.0 or less.
  • Item 2. After the heat-fusible resin layers of the laminate are opposed to each other and heated and pressed in the laminating direction at a temperature of 190 ° C., a surface pressure of 2.0 MPa, and a time of 3 seconds, the thickness of the adhesive layer remains.
  • Item 3. Item 3.
  • Item 4. The battery packaging material according to any one of Items 1 to 3, wherein the adhesive layer has a thickness of 50 ⁇ m or less.
  • Item 5. It is composed of a laminate including at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order, A battery packaging material having a value obtained by measuring the temperature difference T 1 and the temperature difference T 2 by the following method and dividing the temperature difference T 2 by the temperature difference T 1 is 0.60 or more.
  • the heat-fusible resin layer is a solution in which the concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: 1. It is made to dry after leaving still for 72 hours in electrolyte solution which is.
  • a temperature difference T 2 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer after drying is measured.
  • the absolute value of the difference of the temperature difference T 2 and the temperature difference T 1 is is 10 ° C. or less, packaging material for a battery according to claim 5.
  • Item 7. In an environment of 85 ° C., the battery has an electrolyte solution in which the concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: 1.
  • the heat-fusible resin layers are bonded to each other at a temperature of 190 ° C., a surface pressure of 2.0 MPa, and a time of 3 hours with the electrolyte attached to the surface of the heat-fusible resin layer.
  • Item 5 or 6 wherein the seal strength when the heat-sealed interface is peeled off for 2 seconds and the heat-sealed interface is peeled is 85% or more of the seal strength when not contacting the electrolyte.
  • Battery packaging material Item 8.
  • the heat-fusible resin layer contains a lubricant
  • the thermally fused interface is peeled off in an environment of a temperature of 25 ° C. and a relative humidity of 50% under the conditions of a tensile speed of 300 mm / min, a peeling angle of 180 °, and a distance between chucks of 50 mm.
  • Item 10 The battery packaging material according to Item 9, wherein when the tensile strength is measured, the tensile strength is maintained at 100 N / 15 mm or more for 1.5 seconds from 1 second after the start of tensile strength measurement.
  • JIS B0659-1 2002 Annex 1 (reference) A stainless steel plate having a Rz (maximum height roughness) of 0.8 ⁇ m as defined in Table 2 of a comparative surface roughness standard piece, and the heat-fusibility Item 11.
  • the battery packaging material according to Item 9 or 10 wherein the coefficient of dynamic friction with the resin layer is 0.2 or less.
  • Item 12. Item 12.
  • Item 13 Item 13.
  • Item 15. The battery packaging material according to any one of Items 1 to 14, wherein the barrier layer is composed of an aluminum alloy foil or a stainless steel foil.
  • Item 16. At least a method for producing a battery packaging material comprising a step of obtaining a laminate by laminating a base layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order, The adhesive layer is a method for producing a packaging material for a battery, wherein a logarithmic decay rate ⁇ E at 120 ° C. in a rigid pendulum measurement is 2.0 or less.
  • the temperature difference T 1 and the temperature difference T 2 are measured by the following method, and the value obtained by dividing the temperature difference T 2 by the temperature difference T 1 is 0.60 or more.
  • the manufacturing method of the packaging material for batteries. Measurement of temperature difference T 1
  • a temperature difference T 1 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer is measured.
  • the heat-fusible resin layer is a solution in which the concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: 1.
  • the battery packaging material is allowed to stand for 72 hours in an electrolytic solution, and then dried.
  • a temperature difference T 2 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer after drying is measured. Item 18.
  • At least a method for producing a battery packaging material comprising a step of obtaining a laminate by laminating a base material layer, a barrier layer, and a heat-fusible resin layer in this order,
  • the heat-fusible resin layer contains a lubricant
  • the heat-fusible resin layer is a method for producing a packaging material for a battery, wherein a tensile elastic modulus measured according to JIS K7161: 2014 is in a range of 500 MPa to 1000 MPa.
  • Item 19. 16 A battery, wherein a battery element comprising at least a positive electrode, a negative electrode, and an electrolyte is accommodated in a package formed of the battery packaging material according to any one of Items 1 to 15.
  • a battery packaging material composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order. It is possible to provide a battery packaging material that effectively suppresses crushing of the adhesive layer when the heat-resistant resin layers are heat-sealed and exhibits high sealing strength in a high temperature environment. Moreover, according to the 1st aspect of this invention, the manufacturing method of the said packaging material for batteries and the battery using the said packaging material for batteries can also be provided.
  • a battery packaging material comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order. Even when the heat-fusible resin layers are heat-sealed with the electrolyte layer in contact with the resin layer and the electrolyte solution is attached to the heat-fusible resin layer, high sealing strength is exhibited by heat-sealing.
  • a battery packaging material can be provided.
  • the manufacturing method of the said packaging material for batteries and the battery using the said packaging material for batteries can also be provided.
  • a battery packaging material composed of a laminate comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order, contamination of the mold during molding It is possible to provide a battery packaging material that is suppressed and exhibits high sealing strength by thermal fusion. Moreover, according to the 3rd aspect of this invention, the manufacturing method of the said packaging material for batteries and the battery using the said packaging material for batteries can also be provided.
  • FIG. 1 shows an example of the cross-section of the packaging material for batteries of the 2nd aspect and 3rd aspect of this invention. It is a schematic diagram for demonstrating the measuring method of seal strength. It is the schematic diagram explaining an example of the process of accommodating a battery element using a film-form battery packaging material.
  • the temperature difference T 1 and the temperature difference T 2 in differential scanning calorimetry is a diagram schematically showing. It is a schematic diagram for demonstrating the measuring method of a dynamic friction coefficient.
  • the graph which shows the relationship between time and tensile strength obtained by the measurement of tensile strength it is a schematic diagram of a state in which a state of 100 N / 15 mm or more is maintained for 1.5 seconds after 1 second from the start of tensile strength measurement. .
  • the battery packaging material according to the first aspect of the present invention is composed of a laminate including at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer in this order. Is characterized in that the logarithmic decay rate ⁇ E at 120 ° C. in the rigid pendulum measurement is 2.0 or less.
  • the adhesive layer is effectively prevented from being crushed when the heat-fusible resin layers are heat-sealed, and in a high-temperature environment. High seal strength is demonstrated.
  • the battery packaging material according to the first aspect of the present invention has a logarithmic decay rate ⁇ E at 120 ° C. in the rigid pendulum measurement. By being 2.0 or less, the significance of exhibiting high seal strength in a high temperature environment of 120 ° C. is significant.
  • the battery packaging material according to the second aspect of the present invention is a battery packaging material composed of a laminate comprising at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order.
  • a value (ratio T 2 / T 1 ) obtained by dividing the temperature difference T 2 by the temperature difference T 1 is 0.60 or more. It is characterized by that.
  • the electrolytic solution comes into contact with the heat-fusible resin layer in a high-temperature environment, and the heat-fusible resin layer is electrolyzed. Even when the heat-sealable resin layers are heat-sealed with the liquid attached, high sealing strength is exhibited by heat-seal.
  • a temperature difference T 1 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer is measured.
  • the measurement of the temperature difference T 1 is different from the measurement of the temperature difference T 2 described below, and the measurement target is a heat-fusible resin layer that has not been subjected to a treatment such as being immersed in an electrolytic solution.
  • the heat-fusible resin layer is a solution in which the concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: 1. It is made to dry after leaving still for 72 hours in electrolyte solution which is. By differential scanning calorimetry, the temperature difference T 2 between the melting peak temperature extrapolation melting start temperature and the extrapolation melting end temperature of the heat-fusible resin layer after drying is measured.
  • the battery packaging material according to the third aspect of the present invention is composed of a laminate including at least a base material layer, a barrier layer, and a heat-fusible resin layer in this order, and the heat-fusible resin.
  • the layer contains a lubricant and is characterized in that the tensile elastic modulus of the heat-fusible resin layer measured in accordance with JIS K7161: 2014 is in the range of 500 MPa to 1000 MPa.
  • the numerical range indicated by “to” means “above” or “below”.
  • the notation of 2 to 15 mm means 2 mm or more and 15 mm or less.
  • the battery packaging material 10 of the first aspect of the present invention includes, for example, a base material layer 1, a barrier layer 3, an adhesive layer 5, and a heat-sealable property as shown in FIG. It is comprised from the laminated body provided with the resin layer 4 in this order.
  • the battery packaging material 10 according to the second and third aspects of the present invention includes at least a base material layer 1, a barrier layer 3, and a heat-fusible resin layer 4, as shown in FIG. 8, for example. It is comprised from the laminated body provided in this order.
  • an adhesive layer 5 may be provided between the barrier layer 3 and the heat-fusible resin layer 4.
  • the base material layer 1 is the outermost layer side, and the heat-fusible resin layer 4 is the innermost layer. That is, when the battery is assembled, the battery element is sealed by heat-sealing the heat-fusible resin layers 4 positioned at the periphery of the battery element to seal the battery element.
  • the battery packaging material 10 of the present invention may include an adhesive layer 2 between the base material layer 1 and the barrier layer 3 as shown in FIG. Furthermore, as shown in FIG. 3, a surface coating layer 6 may be provided on the outside of the base material layer 1 (on the side opposite to the heat-fusible resin layer 4) as necessary.
  • the thickness of the laminate constituting the battery packaging material 10 of the present invention is not particularly limited, but is, for example, 180 ⁇ m or less, preferably 160 ⁇ m or less, preferably 150 ⁇ m or less, more preferably about 60 to 180 ⁇ m, and still more preferably 60 About 160 ⁇ m, more preferably about 60 to 150 ⁇ m.
  • the battery packaging material that exhibits high sealing strength in a high temperature environment while reducing the thickness of the battery packaging material to increase the energy density of the battery. It can be.
  • the heat-sealable resin layers are heat-sealed with each other in a state where the electrolyte is in contact with the heat-sealable resin layer in a high-temperature environment and the electrolyte is attached to the heat-sealable resin layer. Even in such a case, a battery packaging material that exhibits high sealing strength by heat sealing can be obtained. Furthermore, in the third aspect, while reducing the thickness of the battery packaging material to increase the energy density of the battery, contamination of the mold during molding is suppressed, and high sealing strength is exhibited by heat fusion. It can be used as a battery packaging material.
  • a metal plate having a width of 7 mm is used in a state where the heat-fusible resin layers 4 face each other, and a temperature of 190 is measured in the stacking direction from both sides of the test sample.
  • Heat-pressing is performed under the conditions of ° C., surface pressure of 2.0 MPa, and time of 3 seconds to heat-bond the heat-fusible resin layers 4 to each other (see FIGS. 4 and 5).
  • FIG. First from the start of the measurement of tensile strength using a tensile tester in the environment of a temperature of 25 ° C.
  • the maximum value of tensile strength (seal strength) measured by peeling off the heat-sealed interface for 5 seconds is preferably 125 N / 15 mm or more, and more preferably 130 N / 15 mm or more.
  • the upper limit of the tensile strength is, for example, about 200 N / 15 mm or less, and preferable ranges include 125 to 200 N / 15 mm and 130 to 200 N / 15 mm.
  • the type, composition, molecular weight, and the like of the resin constituting the heat-fusible resin layer are adjusted.
  • the maximum value of tensile strength (seal strength) measured by peeling off the heat-sealed interface for 1.5 seconds is preferably 4.0 N / 15 mm or more, and 4.5 N / 15 mm or more. More preferably.
  • the upper limit of the tensile strength is, for example, about 5.0 N / 15 mm or less, and preferable ranges include 4.0 to 5.0 N / 15 mm and 4.5 to 5.0 N / 15 mm.
  • the heat resistant temperature of the separator inside the battery is generally around 120 to 140 ° C. Therefore, in the battery packaging material according to the first aspect of the present invention, the tensile force in a high temperature environment of 140 ° C. is used.
  • the maximum value of the strength (seal strength) satisfies the above value.
  • the type, composition, molecular weight, and the like of the resin constituting the heat-fusible resin layer are adjusted.
  • the tensile test at each temperature is performed in a thermostat, and the test sample is attached to the chuck in a thermostat at a predetermined temperature (25 ° C. or 140 ° C.) for 2 minutes. Hold and start measurement.
  • the battery packaging material according to the second aspect of the present invention is an electrolyte solution (the concentration of lithium hexafluorophosphate is 1 mol / l and the volume of ethylene carbonate, diethyl carbonate, and dimethyl carbonate in an environment of 85 ° C.
  • the heat-fusible resin layers are heat-fused under the conditions of a temperature of 190 ° C., a surface pressure of 2.0 MPa, and a time of 3 seconds with the electrolytic solution adhering to the surface of the heat-fusible resin layer.
  • the seal strength when peeling the fused interface is preferably 85% or more of the seal strength when not brought into contact with the electrolyte (the retention rate of the seal strength is 85% or more), 90% More preferably above is, more preferably 100%.
  • the retention ratio of the seal strength after contact with the electrolytic solution for 120 hours is preferably 85% or more, more preferably 90% or more, and further preferably 100%.
  • tensile strength is measured in the same manner except that the electrolyte solution is not injected into the test sample.
  • the maximum tensile strength until the heat-sealed portion is completely peeled is defined as the seal strength before contact with the electrolyte.
  • the battery packaging material is cut into a rectangle of width (x direction) 100 mm ⁇ length (z direction) 200 mm to obtain a test sample (FIG. 9 a).
  • the test sample is folded at the center in the z direction so that the heat-fusible resin layer side overlaps (FIG. 9b).
  • both ends in the x direction of the folded test sample are sealed by heat sealing (temperature 190 ° C., surface pressure 2.0 MPa, time 3 seconds), and formed into a bag shape having one opening E (FIG. 9c).
  • an electrolytic solution concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: from the opening E of the test sample formed into a bag shape.
  • 6 g of the solution (solution 1) is injected (FIG. 9d), and the end of the opening E is sealed by heat sealing (temperature 190 ° C., surface pressure 2.0 MPa, time 3 seconds) (FIG. 9e).
  • the folded portion of the bag-shaped test sample is turned down, and is left to stand for a predetermined storage time (a time for contact with the electrolyte, 72 hours, 120 hours, etc.) in an environment at a temperature of 85 ° C.
  • the end portion of the test sample is cut (FIG. 9e), and all the electrolyte solution is discharged.
  • the electrolytic solution adhering to the surface of the heat-fusible resin layer the upper and lower surfaces of the test sample are sandwiched between metal plates (7 mm width), the temperature is 190 ° C., the surface pressure is 1.0 MPa, and the time is 3 seconds.
  • the heat-fusible resin layers are heat-sealed (FIG. 9f).
  • the test sample is cut to a width of 15 mm with a double-edged sample cutter so that the seal strength at a width (x direction) of 15 mm can be measured (FIGS. 9f and 9g).
  • the interface that was heat-sealed was peeled off under the conditions of a tensile speed of 300 mm / min, a peeling angle of 180 °, and a chuck-to-chuck distance of 50 mm, using a tensile tester.
  • the tensile strength (seal strength) is measured (FIG. 6).
  • the maximum tensile strength until the heat-sealed portion is completely peeled is defined as the seal strength after contact with the electrolytic solution.
  • the battery packaging material according to the third aspect of the present invention has a tensile strength of 100 N / W during 1.5 seconds from the start of the tensile strength measurement when the tensile strength is measured by the following method.
  • the state of 15 mm or more is preferably maintained, the state of 110 to 160 N / 15 mm is more preferably maintained, and the state of 120 to 160 N / 15 mm is still more preferable.
  • the time during which the tensile strength is maintained at 100 N / 15 mm or more from 1 second after the start of the tensile strength measurement may be at least 1.5 seconds, for example, 2 seconds, 3 seconds, 9 seconds. The longer the second, the higher the seal strength.
  • the heat-fusible resin layers 4 of the battery packaging material With the heat-fusible resin layers 4 of the battery packaging material facing each other, the heat-fusible resin layers are heat-fused under conditions of a temperature of 190 ° C., a surface pressure of 1.0 MPa, and a time of 3 seconds. Next, using a tensile tester, at a temperature of 25 ° C. and a relative humidity of 50%, a tensile speed of 300 mm / min, a peeling angle of 180 °, and a distance between chucks of 50 mm for 1.5 seconds or more from the start of tensile strength measurement. Then, the heat-sealed interface is peeled off, and the tensile strength (seal strength (N / 15 mm)) is measured. More specific conditions are those described in the examples.
  • the base material layer 1 is common to the first to third embodiments.
  • the base material layer 1 is a layer located on the outermost layer side.
  • the material for forming the base material layer 1 is not particularly limited as long as it has insulating properties.
  • the material for forming the base material layer 1 include resin films such as polyester resin, polyamide resin, epoxy resin, acrylic resin, fluorine resin, polyurethane resin, silicon resin, phenol resin, polycarbonate, and mixtures and copolymers thereof. Is mentioned.
  • a polyester resin and a polyamide resin are mentioned, More preferably, a biaxially stretched polyester resin and a biaxially stretched polyamide resin are mentioned.
  • polyester resin examples include polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, and copolyester.
  • polyamide resin examples include nylon 6, nylon 66, a copolymer of nylon 6 and nylon 66, nylon 6,10, polyamide MXD6 (polymetaxylylene adipamide), and the like.
  • the base material layer 1 may be formed of a single resin film, but may be formed of two or more resin films in order to improve pinhole resistance and insulation. Specific examples include a multilayer structure in which a polyester film and a nylon film are laminated, a multilayer structure in which a plurality of nylon films are laminated, and a multilayer structure in which a plurality of polyester films are laminated.
  • a multilayer structure a laminate of a biaxially stretched nylon film and a biaxially stretched polyester film, a laminate of a plurality of biaxially stretched nylon films, and a laminate of a plurality of biaxially stretched polyester films The body is preferred.
  • the polyester resin and the polyester resin are laminated, the polyamide resin and the polyamide resin are laminated, or the polyester resin and the polyamide resin are laminated. It is more preferable to use a structure in which polyethylene terephthalate and polyethylene terephthalate are laminated, a structure in which nylon and nylon are laminated, or a structure in which polyethylene terephthalate and nylon are laminated.
  • the polyester resin is difficult to discolor when, for example, the electrolytic solution adheres to the surface, it is preferable to laminate the base material layer 1 so that the polyester resin is located in the outermost layer in the laminated configuration.
  • the thickness of each layer is preferably about 2 to 25 ⁇ m.
  • the base material layer 1 is formed of a multilayer resin film
  • two or more resin films may be laminated via an adhesive component such as an adhesive or an adhesive resin, and the type and amount of the adhesive component used. Is the same as that of the adhesive layer 2 described later.
  • the method for laminating two or more resin films is not particularly limited, and a known method can be adopted, and examples thereof include a dry laminating method, a sandwich laminating method, a coextrusion laminating method, and the like, preferably a dry laminating method. Can be mentioned.
  • a dry laminating method it is preferable to use a polyurethane adhesive as the adhesive layer. At this time, the thickness of the adhesive layer is, for example, about 2 to 5 ⁇ m.
  • a lubricant is preferably attached to the surface of the base material layer 1 from the viewpoint of improving the moldability of the battery packaging material.
  • a lubricant Preferably an amide type lubricant is mentioned.
  • Specific examples of the amide-based lubricant include the same ones as exemplified in the heat-fusible resin layer 4 described later.
  • the amount of the lubricant is not particularly limited, but is preferably about 3 mg / m 2 or more, more preferably about 4 to 15 mg / m 2 , further preferably 5 to 14 mg. / M 2 or so.
  • a lubricant may be contained in the base material layer 1. Further, the lubricant present on the surface of the base material layer 1 may be obtained by leaching the lubricant contained in the resin constituting the base material layer 1 or by applying a lubricant to the surface of the base material layer 1. It may be.
  • the total thickness of the base material layer 1 is not particularly limited as long as it exhibits a function as a base material, and is, for example, about 3 to 50 ⁇ m, preferably about 10 to 35 ⁇ m.
  • the adhesive layer 2 is common to the first to third embodiments.
  • the adhesive layer 2 is a layer provided between the base material layer 1 and the barrier layer 3 as necessary in order to firmly bond the base material layer 1 and the barrier layer 3.
  • the adhesive layer 2 is formed of an adhesive capable of bonding the base material layer 1 and the barrier layer 3 together.
  • the adhesive used for forming the adhesive layer 2 may be a two-component curable adhesive or a one-component curable adhesive.
  • the bonding mechanism of the adhesive used for forming the adhesive layer 2 is not particularly limited, and may be any of a chemical reaction type, a solvent volatilization type, a heat melting type, and a hot pressure type.
  • adhesive components that can be used to form the adhesive layer 2 include polyester resins such as polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, and copolyester; polyethers Polyurethane adhesives; epoxy resins; phenol resin resins; polyamide resins such as nylon 6, nylon 66, nylon 12, copolymer polyamides; polyolefins such as polyolefins, carboxylic acid modified polyolefins, metal modified polyolefins Resin, polyvinyl acetate resin; cellulose adhesive; (meth) acrylic resin; polyimide resin; urea resin, melamine resin and other amino resins; chloroprene rubber, nitrile rubber, styrene rubber Rubbers such as diene rubber; and silicone resins. These adhesive components may be used individually by 1 type, and may be used in combination of 2 or more type. Among these adhesive components,
  • the thickness of the adhesive layer 2 is not particularly limited as long as it exhibits an adhesion function, but for example, it is about 1 to 10 ⁇ m, preferably about 2 to 5 ⁇ m.
  • the barrier layer 3 is common to the first to third embodiments.
  • the barrier layer 3 is a layer having a function of preventing water vapor, oxygen, light and the like from entering the battery, in addition to improving the strength of the battery packaging material.
  • the barrier layer 3 is preferably a metal layer, that is, a layer formed of metal. Specific examples of the metal constituting the barrier layer 3 include aluminum, stainless steel, and titanium, and preferably aluminum.
  • the barrier layer 3 can be formed by, for example, a metal foil, a metal vapor-deposited film, an inorganic oxide vapor-deposited film, a carbon-containing inorganic oxide vapor-deposited film, a film provided with these vapor-deposited films, etc.
  • the barrier layer is made of, for example, annealed aluminum (JIS H4160: 1994 A8021H-O, JIS H4160: 1994 A8079H-O, JIS H4000: 2014 A8021P-O, JIS H4000: 2014 A8079P-O) and the like are more preferable.
  • examples of the stainless steel foil include austenitic, ferritic, austenitic / ferritic, martensitic, and precipitation hardening stainless steel foils. Furthermore, from the viewpoint of providing a battery packaging material with excellent formability, the stainless steel foil is preferably made of austenitic stainless steel.
  • austenitic stainless steel constituting the stainless steel foil include SUS304, SUS301, SUS316L, and among these, SUS304 is particularly preferable.
  • the thickness of the barrier layer 3 is not particularly limited as long as it exhibits a barrier function such as water vapor, but is preferably about 100 ⁇ m or less, more preferably about 10 to 100 ⁇ m, from the viewpoint of reducing the thickness of the battery packaging material. More preferably, it is about 10 to 80 ⁇ m, more preferably about 20 to 50 ⁇ m, and still more preferably about 30 to 50 ⁇ m.
  • the barrier layer 3 is preferably subjected to chemical conversion treatment on at least one side, preferably both sides, in order to stabilize adhesion, prevent dissolution and corrosion, and the like.
  • the chemical conversion treatment refers to a treatment for forming an acid-resistant film on the surface of the barrier layer.
  • chromate treatment using a chromium compound such as chromium nitrate, chromium fluoride, chromium sulfate, chromium acetate, chromium oxalate, chromium biphosphate, chromic acid acetyl acetate, chromium chloride, potassium sulfate chromium; Phosphoric acid treatment using a phosphoric acid compound such as sodium phosphate, potassium phosphate, ammonium phosphate, polyphosphoric acid; an aminated phenol polymer having a repeating unit represented by the following general formulas (1) to (4) is used And chromate treatment.
  • the repeating units represented by the following general formulas (1) to (4) may be contained singly or in any combination of two or more. Also good.
  • X represents a hydrogen atom, a hydroxy group, an alkyl group, a hydroxyalkyl group, an allyl group or a benzyl group.
  • R 1 and R 2 are the same or different and each represents a hydroxy group, an alkyl group, or a hydroxyalkyl group.
  • examples of the alkyl group represented by X, R 1 and R 2 include a methyl group, an ethyl group, an n-propyl group, an isopropyl group, an n-butyl group, an isobutyl group, Examples thereof include straight-chain or branched alkyl groups having 1 to 4 carbon atoms such as a tert-butyl group.
  • Examples of the hydroxyalkyl group represented by X, R 1 and R 2 include a hydroxymethyl group, a 1-hydroxyethyl group, a 2-hydroxyethyl group, a 1-hydroxypropyl group, a 2-hydroxypropyl group, 3- Linear or branched chain having 1 to 4 carbon atoms substituted with one hydroxy group such as hydroxypropyl group, 1-hydroxybutyl group, 2-hydroxybutyl group, 3-hydroxybutyl group, 4-hydroxybutyl group An alkyl group is mentioned.
  • the alkyl group and hydroxyalkyl group represented by X, R 1 and R 2 may be the same or different.
  • X is preferably a hydrogen atom, a hydroxy group or a hydroxyalkyl group.
  • the number average molecular weight of the aminated phenol polymer having a repeating unit represented by the general formulas (1) to (4) is preferably about 500 to 1,000,000, for example, about 1,000 to 20,000. More preferred.
  • a phosphoric acid is coated with a metal oxide such as aluminum oxide, titanium oxide, cerium oxide, tin oxide, or barium sulfate fine particles dispersed therein.
  • a method of forming an acid-resistant film on the surface of the barrier layer 3 by performing a baking treatment at 150 ° C. or higher can be mentioned.
  • a resin layer obtained by crosslinking a cationic polymer with a crosslinking agent may be further formed on the acid resistant film.
  • examples of the cationic polymer include polyethyleneimine, an ionic polymer complex composed of a polymer having polyethyleneimine and a carboxylic acid, a primary amine graft acrylic resin obtained by graft polymerization of a primary amine on an acrylic main skeleton, and polyallylamine. Or the derivative, aminophenol, etc. are mentioned.
  • these cationic polymers only one type may be used, or two or more types may be used in combination.
  • examples of the crosslinking agent include a compound having at least one functional group selected from the group consisting of an isocyanate group, a glycidyl group, a carboxyl group, and an oxazoline group, and a silane coupling agent. As these crosslinking agents, only one type may be used, or two or more types may be used in combination.
  • At least the surface on the inner layer side of the aluminum alloy foil is firstly immersed in an alkali soaking method, electrolytic cleaning method, acid cleaning method, electrolytic acid cleaning method.
  • Treatment liquid (aqueous solution) mainly composed of a mixture of metal salts, or treatment liquid (aqueous solution) principally composed of a non-metallic phosphate and a mixture of these non-metallic salts, or acrylic resin Coating a treatment liquid (aqueous solution) consisting of a mixture with a water-based synthetic resin such as phenolic resin or urethane resin by a well-known coating method such as roll coating, gravure printing, or dipping.
  • the acid-resistant coating For example, when treated with a chromium phosphate salt treatment solution, it becomes an acid-resistant film made of chromium phosphate, aluminum phosphate, aluminum oxide, aluminum hydroxide, aluminum fluoride, etc., and treated with a zinc phosphate salt treatment solution. In this case, an acid-resistant film made of zinc phosphate hydrate, aluminum phosphate, aluminum oxide, aluminum hydroxide, aluminum fluoride or the like is obtained.
  • an acid-resistant film for example, at least the surface on the inner layer side of the aluminum alloy foil is first subjected to an alkali dipping method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, an acid An acid-resistant film can be formed by performing a degreasing process by a known processing method such as an activation method and then performing a known anodizing process on the degreasing surface.
  • acid-resistant films include phosphate-based and chromic acid-based films.
  • phosphate-based and chromic acid-based films examples include zinc phosphate, iron phosphate, manganese phosphate, calcium phosphate, and chromium phosphate.
  • chromic acid system examples include chromium chromate.
  • an acid-resistant film by forming an acid-resistant film such as phosphate, chromate, fluoride, triazine thiol compound, between the aluminum and the base material layer at the time of embossing molding
  • an acid-resistant film such as phosphate, chromate, fluoride, triazine thiol compound
  • hydrogen fluoride generated by the reaction between electrolyte and moisture prevents dissolution and corrosion of the aluminum surface, especially the dissolution and corrosion of aluminum oxide present on the aluminum surface, and adhesion of the aluminum surface This improves the wettability and prevents delamination between the base material layer and aluminum at the time of heat fusion.
  • embossed type it shows the effect of preventing delamination between the base material layer and aluminum at the time of press molding.
  • an aqueous solution composed of three components of a phenol resin, a chromium (III) fluoride compound, and phosphoric acid is applied to the aluminum surface, and the dry baking treatment is good.
  • the acid-resistant film includes a layer having cerium oxide, phosphoric acid or phosphate, an anionic polymer, and a crosslinking agent that crosslinks the anionic polymer, and the phosphoric acid or phosphate is About 1 to 100 parts by mass may be blended with 100 parts by mass of cerium oxide. It is preferable that the acid-resistant film has a multilayer structure further including a layer having a cationic polymer and a crosslinking agent for crosslinking the cationic polymer.
  • the anionic polymer is poly (meth) acrylic acid or a salt thereof, or a copolymer containing (meth) acrylic acid or a salt thereof as a main component.
  • the said crosslinking agent is at least 1 sort (s) chosen from the group which has a functional group in any one of an isocyanate group, a glycidyl group, a carboxyl group, and an oxazoline group, and a silane coupling agent.
  • the phosphoric acid or phosphate is preferably condensed phosphoric acid or condensed phosphate.
  • the chemical conversion treatment only one type of chemical conversion treatment may be performed, or two or more types of chemical conversion processing may be performed in combination. Furthermore, these chemical conversion treatments may be carried out using one kind of compound alone, or may be carried out using a combination of two or more kinds of compounds.
  • a chromate treatment a chemical conversion treatment combining a chromium compound, a phosphate compound, and an aminated phenol polymer are preferable.
  • chromium compounds chromic acid compounds are preferred.
  • the acid resistant film examples include those containing at least one of phosphate, chromate, fluoride, and triazine thiol.
  • An acid resistant film containing a cerium compound is also preferable.
  • cerium compound cerium oxide is preferable.
  • the acid resistant film examples include a phosphate film, a chromate film, a fluoride film, and a triazine thiol compound film.
  • a phosphate film As an acid-resistant film, one of these may be used, or a plurality of combinations may be used.
  • a treatment solution comprising a mixture of a metal phosphate and an aqueous synthetic resin, or a mixture of a non-metal phosphate and an aqueous synthetic resin It may be formed of a treatment liquid consisting of
  • the composition of the acid resistant film can be analyzed using, for example, time-of-flight secondary ion mass spectrometry.
  • time-of-flight secondary ion mass spectrometry for example, a peak derived from at least one of Ce + and Cr + is detected.
  • the surface of the aluminum alloy foil is provided with an acid resistant film containing at least one element selected from the group consisting of phosphorus, chromium and cerium.
  • the acid-resistant film on the surface of the aluminum alloy foil of the battery packaging material contains at least one element selected from the group consisting of phosphorus, chromium and cerium. can do. Specifically, first, in the battery packaging material, the heat-fusible resin layer, the adhesive layer, and the like laminated on the aluminum alloy foil are physically peeled off. Next, the aluminum alloy foil is put in an electric furnace, and organic components present on the surface of the aluminum alloy foil are removed at about 300 ° C. for about 30 minutes. Then, it confirms that these elements are contained using the X-ray photoelectron spectroscopy of the surface of aluminum alloy foil.
  • the amount of the acid-resistant film to be formed on the surface of the barrier layer 3 in the chemical conversion treatment is not particularly limited.
  • the chromium compound is chromium per 1 m 2 of the surface of the barrier layer 3.
  • About 0.5 to 50 mg in terms of conversion preferably about 1.0 to 40 mg, about 0.5 to 50 mg, preferably about 1.0 to 40 mg in terms of phosphorus, and about 1.0 to 40 mg of aminated phenol polymer. It is desirable that it is contained in a proportion of about 200 mg, preferably about 5.0 to 150 mg.
  • the thickness of the acid-resistant film is not particularly limited, but is preferably about 1 nm to 10 ⁇ m, more preferably 1 to 1 in terms of the cohesive strength of the film and the adhesion with the barrier layer 3 and the heat-fusible resin layer.
  • the thickness is about 100 nm, more preferably about 1 to 50 nm.
  • the thickness of the acid-resistant film can be measured by observation with a transmission electron microscope or a combination of observation with a transmission electron microscope and energy dispersive X-ray spectroscopy or electron beam energy loss spectroscopy.
  • a solution containing a compound used for forming an acid-resistant film is applied to the surface of the barrier layer by a bar coating method, a roll coating method, a gravure coating method, a dipping method, etc., and then the temperature of the barrier layer is 70. It is performed by heating to about 200 ° C.
  • the barrier layer may be previously subjected to a degreasing treatment by an alkali dipping method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, or the like. By performing the degreasing process in this manner, it is possible to more efficiently perform the chemical conversion process on the surface of the barrier layer.
  • Heat-fusion resin layer 4 Regarding the heat-fusible resin layer 4, items common to the first to third embodiments will be described first, and items unique to each embodiment will be described as respective items.
  • the heat-fusible resin layer 4 corresponds to the innermost layer and is a layer that heat-fuses the heat-fusible resin layers and seals the battery element when the battery is assembled.
  • the resin component used for the heat-fusible resin layer 4 is not particularly limited as long as it can be heat-sealed, and examples thereof include polyolefin, cyclic polyolefin, acid-modified polyolefin, and acid-modified cyclic polyolefin. That is, the heat-fusible resin layer 4 may include a polyolefin skeleton, and preferably includes a polyolefin skeleton. The fact that the heat-fusible resin layer 4 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited.
  • a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the peak may be small and may not be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • polystyrene resin examples include polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, and linear low density polyethylene; homopolypropylene, block copolymer of polypropylene (for example, block copolymer of propylene and ethylene), polypropylene Polypropylenes such as random copolymers of (for example, random copolymers of propylene and ethylene); ethylene-butene-propylene terpolymers, and the like.
  • polyethylene and polypropylene are preferable.
  • the cyclic polyolefin is a copolymer of an olefin and a cyclic monomer, and examples of the olefin that is a constituent monomer of the cyclic polyolefin include ethylene, propylene, 4-methyl-1-pentene, butadiene, and isoprene. .
  • examples of the cyclic monomer that is a constituent monomer of the cyclic polyolefin include cyclic alkenes such as norbornene; specifically, cyclic dienes such as cyclopentadiene, dicyclopentadiene, cyclohexadiene, and norbornadiene.
  • a cyclic alkene is preferable, and norbornene is more preferable.
  • the acid-modified polyolefin is a polymer obtained by modifying the polyolefin by block polymerization or graft polymerization with an acid component such as carboxylic acid.
  • an acid component such as carboxylic acid.
  • the acid component used for modification include carboxylic acids such as maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, and itaconic anhydride, or anhydrides thereof.
  • the acid-modified cyclic polyolefin is obtained by copolymerizing a part of the monomer constituting the cyclic polyolefin in place of the ⁇ , ⁇ -unsaturated carboxylic acid or its anhydride, or by ⁇ , ⁇ - It is a polymer obtained by block polymerization or graft polymerization of an unsaturated carboxylic acid or its anhydride.
  • the cyclic polyolefin to be modified with carboxylic acid is the same as described above.
  • the carboxylic acid used for modification is the same as the acid component used for modification of the polyolefin.
  • polyolefins such as polypropylene and carboxylic acid-modified polyolefins; and more preferred are polypropylene and acid-modified polypropylene.
  • the heat-fusible resin layer 4 may be formed of one kind of resin component alone or may be formed of a blend polymer in which two or more kinds of resin components are combined. Furthermore, the heat-fusible resin layer 4 may be formed of only one layer, but may be formed of two or more layers using the same or different resin components.
  • a lubricant may be contained in the heat-fusible resin layer 4. Further, the lubricant present on the surface of the heat-fusible resin layer 4 may be one in which a lubricant contained in the resin constituting the heat-fusible resin layer 4 is exuded, or the heat-fusible resin layer. 4 may be obtained by applying a lubricant to the surface.
  • the heat-fusible resin layer 4 contains a lubricant.
  • the lubricant may be present in the heat-fusible resin layer 4, may be present on the surface, or both. May be present.
  • the lubricant is not particularly limited, but preferably an amide lubricant.
  • Specific examples of the amide-based lubricant include saturated fatty acid amide, unsaturated fatty acid amide, substituted amide, methylolamide, saturated fatty acid bisamide, unsaturated fatty acid bisamide, and the like.
  • Specific examples of the saturated fatty acid amide include lauric acid amide, palmitic acid amide, stearic acid amide, behenic acid amide, hydroxy stearic acid amide and the like.
  • Specific examples of the unsaturated fatty acid amide include oleic acid amide and erucic acid amide.
  • substituted amide examples include N-oleyl palmitic acid amide, N-stearyl stearic acid amide, N-stearyl oleic acid amide, N-oleyl stearic acid amide, N-stearyl erucic acid amide and the like.
  • methylolamide examples include methylol stearamide.
  • saturated fatty acid bisamides include methylene bis stearamide, ethylene biscapric amide, ethylene bis lauric acid amide, ethylene bis stearic acid amide, ethylene bishydroxy stearic acid amide, ethylene bisbehenic acid amide, hexamethylene bis stearic acid amide.
  • acid amide hexamethylene bisbehenic acid amide, hexamethylene hydroxystearic acid amide, N, N′-distearyl adipic acid amide, N, N′-distearyl sebacic acid amide, and the like.
  • unsaturated fatty acid bisamides include ethylene bisoleic acid amide, ethylene biserucic acid amide, hexamethylene bisoleic acid amide, N, N′-dioleyl adipic acid amide, N, N′-dioleyl sebacic acid amide Etc.
  • Specific examples of the fatty acid ester amide include stearoamidoethyl stearate.
  • aromatic bisamide examples include m-xylylene bis stearic acid amide, m-xylylene bishydroxy stearic acid amide, N, N′-distearyl isophthalic acid amide and the like.
  • One type of lubricant may be used alone, or two or more types may be used in combination.
  • the amount of the lubricant is not particularly limited, but is preferably about 3 mg / m 2 or more, more preferably about 4 to 15 mg / m 2 , more preferably Examples thereof include about 5 to 14 mg / m 2 .
  • the lubricant present on the surface of the heat-fusible resin layer 4 may be one in which a lubricant contained in the resin constituting the heat-fusible resin layer 4 is exuded. You may apply
  • the thickness of the heat-fusible resin layer 4 is not particularly limited as long as it exhibits the function as the heat-fusible resin layer, but is preferably about 60 ⁇ m or less, more preferably 15 to About 60 ⁇ m, more preferably about 15 to 45 ⁇ m, and still more preferably about 15 to 40 ⁇ m.
  • the temperature difference T 2 is divided by the temperature difference T 1 .
  • the value (ratio T 2 / T 1 ) obtained in this way is 0.60 or more.
  • the ratio T 2 / T 1 is closer to the upper limit of 1.0, the heat-fusible resin layer comes into contact with the electrolytic solution. This means that the change in the width of the melting peak start point (extrapolation melting start temperature) and end point (extrapolation melting end temperature) before and after is small (see the schematic diagram of FIG. 11).
  • the value of T 2 is usually less than or equal to the value of T 1 .
  • the reason for the large change in the range between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak is that the low molecular weight resin contained in the resin constituting the heat-fusible resin layer contacts the electrolyte.
  • the range of the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak of the heat-fusible resin layer after elution into the electrolyte solution and contact with the electrolyte solution is different from that before contact with the electrolyte solution. Then, it can be mentioned that it becomes smaller.
  • Percentage of low molecular weight resin contained in the resin constituting the heat-fusible resin layer as one of the methods for reducing the change in the range of the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak.
  • the method of adjusting is mentioned.
  • a differential scanning calorimetry is used to obtain a DSC curve for the polypropylene used for the heat-fusible resin layer of each of the battery packaging materials. From the obtained DSC curve, the temperature difference T 1 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer is measured.
  • the polypropylene used for the heat-fusible resin layer has a lithium hexafluorophosphate concentration of 1 mol / l and a volume ratio of ethylene carbonate, diethyl carbonate and dimethyl carbonate of 1: 1: After leaving still for 72 hours in the electrolyte solution which is 1 solution, it fully dries.
  • a DSC curve is obtained for the dried polypropylene using differential scanning calorimetry (DSC) in accordance with JIS K7121: 2012.
  • DSC differential scanning calorimetry
  • the differential scanning calorimeter shows that the test sample was held at ⁇ 50 ° C. for 10 minutes, then heated to 200 ° C. at the temperature rising rate of 10 ° C./min (first time), held at 200 ° C. for 10 minutes, and then the temperature decreasing rate The temperature was lowered to ⁇ 50 ° C. at ⁇ 10 ° C./min, held at ⁇ 50 ° C. for 10 minutes, then heated to 200 ° C. at the rate of temperature increase of 10 ° C./min (second time), held at 200 ° C.
  • the DSC curve when the temperature is raised to 200 ° C. for the second time is used. Also, when measuring the temperature difference T 1 and temperature difference T 2 , analyze the melting peak that maximizes the difference in thermal energy input among the melting peaks that appear in the range of 120 to 160 ° C in each DSC curve. Do. Even when two or more peaks overlap, the analysis is performed only for the melting peak that maximizes the difference in the input of thermal energy.
  • the extrapolated melting start temperature means the starting point of the melting peak temperature, and the melting that maximizes the difference between the heat energy input and the straight line obtained by extending the base line on the low temperature (65 to 75 ° C) side to the high temperature side.
  • the temperature at the intersection of the tangent drawn on the curve on the low temperature side of the peak at the point where the gradient is maximum is taken.
  • Extrapolation end temperature means the end of the melting peak temperature, and the high temperature side of the melting peak where the difference between the heat energy input and the straight line obtained by extending the base line on the high temperature (170 ° C) side to the low temperature side becomes the maximum.
  • the heat-sealable resin layers are heat-sealed with each other in a state where the electrolyte is in contact with the heat-sealable resin layer in a high temperature environment and the electrolyte is attached to the heat-sealable resin layer.
  • the value (ratio T 2 / T 1 ) obtained by dividing the temperature difference T 2 by the temperature difference T 1 is preferable from the viewpoint of exhibiting a higher seal strength by heat fusion.
  • Is 0.70 or more, more preferably 0.75 or more, and preferable ranges are about 0.70 to 1.0 and about 0.75 to 1.0.
  • the upper limit is 1.0, for example.
  • the ratio T 2 / T 1 for example, the type, composition, molecular weight, and the like of the resin constituting the heat-fusible resin layer 4 are adjusted.
  • the heat-fusible resin layers are heat-sealed with each other in a state where the electrolyte solution is in contact with the heat-fusible resin layer in a high temperature environment and the electrolyte solution is attached to the heat-fusible resin layer.
  • of the difference between the temperature difference T 2 and the temperature difference T 1 is preferably about 10 ° C. from the viewpoint of exhibiting a higher seal strength by thermal fusion. In the following, more preferably about 8 ° C. or less, still more preferably about 7.5 ° C.
  • the temperature is about 5 to 7.5 ° C.
  • of the difference is, for example, 0 ° C., 1 ° C., 2 ° C., 5 ° C., or the like. In order to set the absolute value
  • the temperature difference T 1 is preferably about 31 to 38 ° C., more preferably about 32 to 36 ° C.
  • the temperature difference T 2 is preferably about 25 to 30 ° C., more preferably about 26 to 29 ° C.
  • the type, composition, molecular weight, and the like of the resin constituting the heat-fusible resin layer 4 are adjusted.
  • the extrapolation start temperature of the melting peak temperature of the heat-fusible resin layer in the measurement of the temperature difference T 1 is, for example, about 123 to 130 ° C. Is about 156 to 165 ° C., for example. Further, the extrapolation start temperature of the melting peak temperature of the heat-fusible resin layer in the measurement of the temperature difference T 1 is, for example, about 125 to 132 ° C., and the extrapolation end temperature is, for example, 151 to 160. A temperature of about ° C can be mentioned.
  • the heat-fusible resin layer 4 contains a lubricant from the viewpoint of improving the moldability of the battery packaging material.
  • the lubricant may be present in the heat-fusible resin layer 4, may be present on the surface, or both. May be present.
  • the same lubricant as that exemplified in the first embodiment is preferably exemplified.
  • the amount of the lubricant is not particularly limited, but is preferably about 3 mg / m 2 or more, more preferably about 4 to 15 mg / m 2 , more preferably Examples thereof include about 5 to 14 mg / m 2 .
  • the lubricant present on the surface of the heat-fusible resin layer 4 may be one in which a lubricant contained in the resin constituting the heat-fusible resin layer 4 is exuded. You may apply
  • the thickness of the heat-fusible resin layer 4 is not particularly limited as long as it exhibits the function as the heat-fusible resin layer.
  • the lower limit is preferably about 10 ⁇ m or more, more preferably about 15 ⁇ m or more
  • the upper limit is preferably about 60 ⁇ m or less, more preferably about 45 ⁇ m or less.
  • Preferable ranges of the thickness of the heat-fusible resin layer include about 10 to 60 ⁇ m, about 10 to 45 ⁇ m, about 15 to 60 ⁇ m, and about 15 to 45 ⁇ m.
  • the heat-fusible resin layer 4 contains a lubricant, and the tensile elastic modulus of the heat-fusible resin layer 4 is 500 to 1000 MPa. It is characterized by being in range.
  • a mold for molding a battery packaging material it has a high surface smoothness (for example, JIS B 0659-1: 2002, Annex 1 (reference). When a mold made of stainless steel) is used, the contact area between the mold and the heat-fusible resin layer 4 is increased.
  • the lubricant located on the surface of the fusible resin layer 4 is easily scraped, the lubricant located on the surface portion of the heat fusible resin layer 4 is easily transferred to the mold, contaminates the mold, and continuously produces batteries. There is a problem that the performance is lowered.
  • the battery packaging material according to the third aspect of the present invention since the tensile elastic modulus of the heat-fusible resin layer 4 is within such a specific range, gold having high surface smoothness is obtained.
  • the lubricant located on the surface of the heat-fusible resin layer 4 is difficult to be scraped, so that contamination of the mold during molding of the battery packaging material is suppressed, and high sealing by heat-sealing Can exhibit strength.
  • the tensile elastic modulus of the heat-fusible resin layer 4 is 500 MPa or more, contamination of the mold during molding is effectively suppressed. That is, when the tensile elastic modulus of the heat-fusible resin layer 4 is 500 MPa or more, the lubricant located on the surface of the heat-fusible resin layer 4 is difficult to be scraped off by the mold.
  • the lubricant located on the surface portion of the mold is difficult to transfer to the mold, and contamination of the mold is effectively suppressed.
  • the tensile elastic modulus of the heat-fusible resin layer 4 is 1000 MPa or less, high sealing strength is exhibited by heat-sealing. That is, since the heat-fusible resin layer 4 is less likely to become brittle when the tensile elastic modulus of the heat-fusible resin layer 4 is 1000 MPa or less, high seal strength is exhibited by heat-sealing.
  • the heat-fusible resin layer 4 When the tensile elastic modulus of the heat-fusible resin layer 4 exceeds 1000 MPa, the heat-fusible resin layer 4 tends to become brittle and easily peels from the barrier layer 3 laminated via the adhesive layer 5, thereby providing a sealing strength. Decrease, or whitening or cracking occurs in the stretched part due to stretching in the cold forming process, resulting in a decrease in battery performance. Moreover, since the extrudability will fall when the tensile elasticity modulus of the heat-fusible resin layer 4 exceeds 1000 MPa, it becomes a factor that productivity falls.
  • the tensile elasticity modulus of the heat-fusible resin layer 4 is in the range of 500 to 1000 MPa, so that the effect of suppressing mold contamination and the improvement of the sealing strength by heat-sealing are achieved. An effect is exhibited suitably.
  • the tensile elasticity modulus of the heat-fusible resin layer 4 can be adjusted by adjusting the molecular weight of the resin constituting the heat-fusible resin layer 4, the melt mass flow rate (MFR), and the like.
  • the tensile modulus of the heat-fusible resin layer 4 is from the viewpoint of exhibiting higher sealing strength by heat fusion while more effectively suppressing contamination of the mold during molding.
  • the kind of resin which comprises the heat-fusible resin layer 4, a composition, molecular weight, etc. are adjusted, for example.
  • the tensile elastic modulus of the heat-fusible resin layer 4 is a value measured in accordance with JIS K7161: 2014.
  • the heat-fusible resin layer 4 and a stainless steel plate As a dynamic friction coefficient with Rz (maximum height roughness) of 0.8 ⁇ m provided in Table 2 of Comparative Surface Roughness Standard Piece, preferably 0 .25 or less, more preferably 0.20 or less, and still more preferably 0.17 or less.
  • 0.08 is mentioned as a minimum of a dynamic friction coefficient.
  • Preferable ranges of the dynamic friction coefficient include about 0.08 to 0.25, about 0.08 to 0.20, and about 0.08 to 0.17. A specific method for measuring the dynamic friction coefficient is shown in the examples.
  • the heat-fusible resin layer 4 contains a lubricant, and when the battery packaging material of the third aspect is used for molding, the surface of the heat-fusible resin layer 4 There is a lubricant.
  • the amount of lubricant present on the surface of the heat-fusible resin layer 4 is not particularly limited, but is preferably about 3 mg / m 2 or more, more preferably about 4 to 15 mg / m 2 , and still more preferably 5 to 14 mg / m 2. There are about two .
  • the amount of lubricant present on the surface of the heat-fusible resin layer 4 can be suitably adjusted to 0.25 or less.
  • the amount of lubricant on the surface of the heat-fusible resin layer or the base material layer is determined by washing a predetermined area on the surface of the heat-fusible resin layer or the base material layer with a solvent, respectively, in the obtained cleaning liquid (solvent).
  • the amount of lubricant contained can be quantified using a gas chromatograph mass spectrometer (GC-MS).
  • the same lubricants as exemplified in the first embodiment are preferably exemplified.
  • the lubricant present on the surface of the heat-fusible resin layer 4 may be one in which a lubricant contained in the resin constituting the heat-fusible resin layer 4 is exuded. You may apply
  • the thickness of the heat-fusible resin layer 4 is not particularly limited as long as it exhibits the function as the heat-fusible resin layer.
  • the heat-sealing resin layer 4 exhibits even higher sealing strength.
  • the lower limit is preferably about 30 ⁇ m or more, more preferably about 35 ⁇ m or more
  • the upper limit is preferably about 60 ⁇ m or less, more preferably about 45 ⁇ m or less.
  • Preferable ranges of the thickness of the heat-fusible resin layer include about 30 to 60 ⁇ m, about 30 to 45 ⁇ m, about 35 to 60 ⁇ m, and about 35 to 45 ⁇ m.
  • the adhesive layer 5 firmly bonds the barrier layer 3 and the heat-fusible resin layer 4 and is highly sealed in a high temperature environment. It is a layer provided for exerting strength.
  • the adhesive layer 5 is a layer provided between the barrier layer 3 and the heat-fusible resin layer 4 as necessary in order to firmly bond the barrier layer 3 and the heat-fusible resin layer 4. .
  • the adhesive layer 5 is characterized in that the logarithmic decay rate ⁇ E at 120 ° C. in the rigid pendulum measurement is 2.0 or less.
  • the logarithmic decay rate ⁇ E at 120 ° C. is 2.0 or less
  • the heat-fusible resin layers are heat-sealed. Crushing of the adhesive layer is effectively suppressed, and high sealing strength in a high temperature environment is exhibited.
  • the logarithmic decay rate at 120 ° C. in the rigid pendulum measurement is an index representing the hardness of the resin in a high temperature environment of 120 ° C., and the smaller the logarithmic decay rate, the higher the hardness of the resin.
  • the attenuation rate of the pendulum is measured when the temperature of the resin is raised from a low temperature to a high temperature.
  • the edge portion is brought into contact with the surface of the measurement object, and the pendulum is moved in the left-right direction to impart vibration to the measurement object.
  • the hard adhesive layer 5 having a logarithmic decay rate of 2.0 or less in a high temperature environment of 120 ° C.
  • ⁇ E [ln (A1 / A2) + ln (A2 / A3) +... Ln (An / An + 1)] / n A: Amplitude n: Wave number
  • the adhesive layer 5 is effectively prevented from being crushed when the heat-fusible resin layers 4 are heat-sealed, and the sealing strength is high in a high-temperature environment.
  • the logarithmic decay rate ⁇ E at 120 ° C. is preferably about 1.4 to 2.0, more preferably about 1.4 to 1.6.
  • the type, composition, molecular weight, and the like of the resin constituting the adhesive layer 5 are adjusted.
  • a commercially available rigid pendulum type physical property tester is used, a cylindrical cylinder edge as an edge portion pressed against the adhesive layer 5, an initial amplitude of 0.3 degree, and a temperature of 30 ° C. to 200 ° C.
  • a rigid pendulum physical property test is performed on the adhesive layer 5 at a temperature rising rate of 3 ° C./min. Then, based on the logarithmic decay rate at 120 ° C., the criteria for suppressing the crushing exerted by the adhesive layer 5 and the effect of improving the seal strength by thermal fusion in a high temperature environment were determined.
  • the battery packaging material was immersed in 15% hydrochloric acid to dissolve the base material layer and the aluminum foil, and only the adhesive layer and the heat-fusible resin layer were obtained. The sample is sufficiently dried to be measured.
  • the heat-fusible resin layer of the laminate constituting the battery packaging material is opposed, the temperature is 190 ° C., the surface pressure is 2.0 MPa, and the time is After heating and pressing in the laminating direction for 3 seconds, the residual ratio of the thickness of the adhesive layer is preferably 40% or more, more preferably 42% or more, and more preferably 45% or more. Preferable ranges include 40 to 50%, 42 to 50%, and 45 to 50%. In addition, the upper limit of the residual ratio of the thickness is usually about 50%. The residual ratio of the thickness is a value measured by the following method.
  • the remaining ratio of the thickness of the adhesive layer If it is 40% or more, it can be evaluated that the adhesive layer when the heat-fusible resin layers are heat-sealed is effectively suppressed.
  • the remaining ratio of the thickness for example, the type, composition, molecular weight, and the like of the resin constituting the adhesive layer 5 are adjusted.
  • the battery packaging material is cut into a length of 150 mm and a width of 60 mm to prepare a test sample.
  • the heat-fusible resin layers of the test sample are opposed to each other.
  • heat and pressure are applied from both sides of the test sample in the laminating direction under conditions of a temperature of 190 ° C., a surface pressure of 2.0 MPa, and a time of 3 seconds.
  • Heat-sealable resin layers are cut in the stacking direction using a microtome, and the thickness of the adhesive layer is measured for the exposed cross section.
  • test sample before heat sealing is cut in the stacking direction using a microtome, and the thickness of the adhesive layer is measured for the exposed cross section.
  • the ratio of the thickness of the adhesive layer after heat fusion to the thickness of the adhesive layer before heat fusion is calculated, and the remaining ratio (%) of the thickness of the adhesive layer is measured.
  • a battery packaging material can be obtained from the battery, and the remaining ratio of the thickness of the adhesive layer 5 can be measured.
  • the battery packaging material is obtained from the battery and the remaining ratio of the thickness of the adhesive layer 5 is measured, a sample is cut out from the top surface portion where the battery packaging material is not stretched by molding to be a measurement object.
  • the adhesive layer 5 is formed of a resin capable of bonding the barrier layer 3 and the heat-fusible resin layer 4.
  • the resin constituting the adhesive layer 5 is not particularly limited as long as it has the above-described logarithmic decay rate ⁇ E, but it effectively suppresses the collapse of the adhesive layer when the heat-fusible resin layers are heat-sealed.
  • acid-modified polyolefin is exemplified. That is, in the present invention, the resin constituting the adhesive layer 5 preferably contains an acid-modified polyolefin.
  • the resin constituting the adhesive layer 5 may include a polyolefin skeleton, and preferably includes a polyolefin skeleton.
  • the fact that the resin constituting the adhesive layer 5 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited.
  • infrared spectroscopy when measuring the infrared spectroscopy at a maleic anhydride-modified polyolefin, a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1. However, if the acid modification degree is low, the peak may be small and may not be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • the logarithmic decay rate ⁇ E of the adhesive layer 5 can be adjusted by, for example, the melt mass flow rate (MFR), molecular weight, melting point, softening point, molecular weight distribution, crystallinity, etc. of the resin constituting the adhesive layer 5.
  • MFR melt mass flow rate
  • molecular weight molecular weight
  • melting point melting point
  • softening point molecular weight distribution
  • crystallinity etc.
  • the acid-modified polyolefin is a polymer obtained by block polymerization or graft polymerization of polyolefin with an acid component such as carboxylic acid.
  • an acid component such as carboxylic acid.
  • the acid component used for modification include carboxylic acids such as maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, and itaconic anhydride, or anhydrides thereof.
  • polyolefins include polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, and linear low density polyethylene; homopolypropylene, polypropylene block copolymers (for example, block copolymers of propylene and ethylene), polypropylene Polypropylenes such as random copolymers (eg, random copolymers of propylene and ethylene); ethylene-butene-propylene terpolymers and the like.
  • polyethylene and polypropylene are preferable.
  • the acid-modified cyclic polyolefin is obtained by copolymerizing a part of the monomer constituting the cyclic polyolefin in place of the ⁇ , ⁇ -unsaturated carboxylic acid or its anhydride, or by ⁇ , ⁇ with respect to the cyclic polyolefin.
  • the cyclic polyolefin to be modified with carboxylic acid is a copolymer of an olefin and a cyclic monomer
  • examples of the olefin that is a constituent monomer of the cyclic polyolefin include ethylene, propylene, 4-methyl-1-pentene, butadiene, And isoprene.
  • examples of the cyclic monomer that is a constituent monomer of the cyclic polyolefin include cyclic alkenes such as norbornene; specifically, cyclic dienes such as cyclopentadiene, dicyclopentadiene, cyclohexadiene, and norbornadiene.
  • a cyclic alkene is preferable, and norbornene is more preferable.
  • the carboxylic acid used for modification is the same as the acid component used for modification of the polyolefin.
  • acid-modified polyolefin is preferable, acid-modified polypropylene is more preferable, and maleic anhydride-modified polypropylene is particularly preferable.
  • the adhesive layer 5 of the first aspect may be formed of one kind of resin component alone, or may be formed of a blend polymer in which two or more kinds of resin components are combined.
  • the thickness of the adhesive layer 5 effectively suppresses the collapse of the adhesive layer when the heat-fusible resin layers are heat-sealed to each other, and exhibits high sealing strength in a high-temperature environment. From the viewpoint, it is preferably about 50 ⁇ m or less, more preferably about 2 to 50 ⁇ m, still more preferably about 10 to 45 ⁇ m, and particularly preferably about 20 to 45 ⁇ m.
  • the adhesive layer 5 of the second embodiment and the third embodiment is formed of a resin capable of bonding the barrier layer 3 and the heat-fusible resin layer 4. Is done.
  • the resin used for forming the adhesive layer 5 the same adhesive mechanism and the same types of adhesive components as those exemplified for the adhesive layer 2 can be used.
  • polyolefin resins such as polyolefin, cyclic polyolefin, carboxylic acid-modified polyolefin, carboxylic acid-modified cyclic polyolefin exemplified in the above-mentioned heat-fusible resin layer 4 can also be used. .
  • the polyolefin is preferably a carboxylic acid-modified polyolefin, and particularly preferably a carboxylic acid-modified polypropylene. That is, the adhesive layer 5 may include a polyolefin skeleton, and preferably includes a polyolefin skeleton. The fact that the adhesive layer 5 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited.
  • a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the peak may be small and may not be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • the adhesive layer 5 is an acid layer. It may be a cured product of a resin composition containing a modified polyolefin and a curing agent.
  • Preferred examples of the acid-modified polyolefin include the same carboxylic acid-modified polyolefin and carboxylic acid-modified cyclic polyolefin exemplified in the heat-fusible resin layer 4.
  • the curing agent is not particularly limited as long as it can cure the acid-modified polyolefin.
  • the curing agent include an epoxy curing agent, a polyfunctional isocyanate curing agent, a carbodiimide curing agent, and an oxazoline curing agent.
  • the epoxy curing agent is not particularly limited as long as it is a compound having at least one epoxy group.
  • examples of the epoxy curing agent include epoxy resins such as bisphenol A diglycidyl ether, modified bisphenol A diglycidyl ether, novolac glycidyl ether, glycerin polyglycidyl ether, and polyglycerin polyglycidyl ether.
  • the polyfunctional isocyanate curing agent is not particularly limited as long as it is a compound having two or more isocyanate groups.
  • Specific examples of the polyfunctional isocyanate-based curing agent include isophorone diisocyanate (IPDI), hexamethylene diisocyanate (HDI), tolylene diisocyanate (TDI), diphenylmethane diisocyanate (MDI), those obtained by polymerizing or nurating these, Examples thereof include mixtures and copolymers with other polymers.
  • the carbodiimide curing agent is not particularly limited as long as it is a compound having at least one carbodiimide group (—N ⁇ C ⁇ N—).
  • a polycarbodiimide compound having at least two carbodiimide groups is preferable.
  • the oxazoline-based curing agent is not particularly limited as long as it is a compound having an oxazoline skeleton.
  • Specific examples of the oxazoline-based curing agent include Epocros series manufactured by Nippon Shokubai Co., Ltd.
  • the curing agent is composed of two or more kinds of compounds. May be.
  • the content of the curing agent in the resin composition forming the adhesive layer 5 of the second and third aspects is preferably in the range of about 0.1 to 50% by mass, and 0.1 to 30% by mass. More preferably, it is in the range of about 0.1 to 10% by mass.
  • the thickness of the adhesive layer 5 of the second aspect and the third aspect is not particularly limited as long as it exhibits the function as the adhesive layer, but is preferable if the adhesive exemplified in the adhesive layer 2 is used. Is about 1 to 10 ⁇ m, more preferably about 1 to 5 ⁇ m. Further, when the resin exemplified in the heat-fusible resin layer 4 is used, it is preferably about 2 to 50 ⁇ m, more preferably 10 to 45 ⁇ m, and still more preferably about 20 to 45 ⁇ m.
  • a cured product of an acid-modified polyolefin and a curing agent it is preferably about 30 ⁇ m or less, more preferably about 0.1 to 20 ⁇ m, and still more preferably about 0.5 to 5 ⁇ m.
  • the adhesive layer 5 can be formed by applying the resin composition and curing it by heating or the like.
  • the surface coating layer 6 is common to the first to third embodiments.
  • the base material layer 1 (barrier layer of the base material layer 1) is optionally formed.
  • the surface coating layer 6 may be provided on the side opposite to 3.
  • the surface coating layer 6 is a layer located in the outermost layer when the battery is assembled.
  • the surface coating layer 6 can be formed of, for example, polyvinylidene chloride, polyester resin, urethane resin, acrylic resin, epoxy resin, or the like. Of these, the surface coating layer 6 is preferably formed of a two-component curable resin. Examples of the two-component curable resin for forming the surface coating layer 6 include a two-component curable urethane resin, a two-component curable polyester resin, and a two-component curable epoxy resin. Moreover, you may mix
  • Examples of the additive include fine particles having a particle size of about 0.5 nm to 5 ⁇ m.
  • the material of the additive is not particularly limited, and examples thereof include metals, metal oxides, inorganic substances, and organic substances.
  • the shape of the additive is not particularly limited, and examples thereof include a spherical shape, a fiber shape, a plate shape, an indeterminate shape, and a balloon shape.
  • Specific additives include talc, silica, graphite, kaolin, montmorilloid, montmorillonite, synthetic mica, hydrotalcite, silica gel, zeolite, aluminum hydroxide, magnesium hydroxide, zinc oxide, magnesium oxide, aluminum oxide, Neodymium oxide, antimony oxide, titanium oxide, cerium oxide, calcium sulfate, barium sulfate, calcium carbonate, calcium silicate, lithium carbonate, calcium benzoate, calcium oxalate, magnesium stearate, alumina, carbon black, carbon nanotubes, high Melting
  • money, aluminum, copper, nickel etc. are mentioned.
  • additives may be used individually by 1 type, and may be used in combination of 2 or more type.
  • silica, barium sulfate, and titanium oxide are preferably used from the viewpoint of dispersion stability and cost.
  • the surface of the additive may be subjected to various surface treatments such as insulation treatment and high dispersibility treatment.
  • the content of the additive in the surface coating layer is not particularly limited, but is preferably about 0.05 to 1.0% by mass, more preferably about 0.1 to 0.5% by mass.
  • the method for forming the surface coating layer 6 is not particularly limited, and examples thereof include a method in which a two-component curable resin for forming the surface coating layer 6 is applied to one surface of the base material layer 1.
  • the additive may be added to the two-component curable resin, mixed, and then applied.
  • the thickness of the surface coating layer 6 is not particularly limited as long as the above function as the surface coating layer 6 is exhibited.
  • the thickness is about 0.5 to 10 ⁇ m, preferably about 1 to 5 ⁇ m.
  • the production method for the battery packaging material according to the first aspect of the present invention is not particularly limited as long as a laminate in which layers having a predetermined composition are laminated is obtained. That is, in the method for manufacturing a battery packaging material according to the first aspect of the present invention, at least a base material layer, a barrier layer, an adhesive layer, and a heat-fusible resin layer are laminated in this order. A layered body is obtained, and an adhesive layer having a logarithmic decay rate ⁇ E at 120 ° C. in the rigid pendulum measurement of 2.0 or less is used. The configuration of each layer of the laminate and the logarithmic attenuation factor ⁇ E are as described above.
  • the method for producing a battery packaging material according to the second aspect of the present invention is not particularly limited as long as a laminate in which layers having a predetermined composition are laminated is obtained. That is, in the method for producing a battery packaging material according to the second aspect of the present invention, at least a base material layer, a barrier layer, and a heat-fusible resin layer are laminated in this order. When the temperature difference T 1 and the temperature difference T 2 are measured by the above method as a heat-fusible resin layer, the temperature difference T 2 is divided by the temperature difference T 1. The value obtained is 0.60 or more. About the structure of each layer of a laminated body, it is as above-mentioned.
  • the method for producing the battery packaging material according to the third aspect of the present invention is not particularly limited as long as a laminate in which layers having a predetermined composition are laminated is obtained. That is, in the method for producing a battery packaging material according to the third aspect of the present invention, the laminate is formed by laminating at least the base material layer, the barrier layer, and the heat-fusible resin layer in this order.
  • the heat-fusible resin layer contains a lubricant, and the tensile elastic modulus measured according to JIS K7161: 2014 as the heat-fusible resin layer is 500 MPa or more. The thing in the range of 1000 Mpa or less is used. About the structure of each layer of a laminated body, it is as above-mentioned.
  • a laminate in which the base material layer 1, the adhesive layer 2, and the barrier layer 3 are laminated in this order (hereinafter also referred to as “laminate A”) is formed.
  • the laminate A is formed by applying an adhesive used for forming the adhesive layer 2 to the base material layer 1 or the barrier layer 3 whose surface is subjected to chemical conversion treatment, if necessary, using a gravure coating method, a roll
  • a coating method such as a coating method
  • it can be performed by a dry laminating method in which the barrier layer 3 or the base material layer 1 is laminated and the adhesive layer 2 is cured.
  • the adhesive layer 5 and the heat-fusible resin layer 4 are laminated on the barrier layer 3 of the laminate A in this order.
  • a method of laminating the adhesive layer 5 and the heat-fusible resin layer 4 on the barrier layer 3 of the laminate A by coextrusion (coextrusion laminating method) (2) a separate adhesive layer 5 And a layered product of the heat-fusible resin layer 4 and a method of laminating the layered product on the barrier layer 3 of the layered product A by a thermal laminating method.
  • the adhesive for forming the layer 5 is laminated by an extrusion method, solution coating, drying at a high temperature or baking, and the heat-fusible resin layer 4 previously formed into a sheet on the adhesive layer 5 is formed.
  • the molten adhesive layer 5 is poured between the barrier layer 3 of the laminate A and the heat-fusible resin layer 4 previously formed into a sheet (film) shape.
  • heat-sealing with the laminate A via the adhesive layer 5 A method of bonding the resin layer 4 (sandwich lamination method).
  • the surface coating layer 6 When the surface coating layer 6 is provided, the surface coating layer 6 is laminated on the surface of the base material layer 1 opposite to the barrier layer 3.
  • the surface coating layer 6 can be formed, for example, by applying the above-described resin for forming the surface coating layer 6 to the surface of the base material layer 1.
  • the order of the step of laminating the barrier layer 3 on the surface of the base material layer 1 and the step of laminating the surface coating layer 6 on the surface of the base material layer 1 are not particularly limited.
  • the barrier layer 3 may be formed on the surface of the base material layer 1 opposite to the surface coating layer 6.
  • each layer constituting the laminate improves or stabilizes film forming properties, lamination processing, suitability for final processing of secondary products (pouching, embossing), and the like as necessary. Therefore, surface activation treatment such as corona treatment, blast treatment, oxidation treatment, ozone treatment may be performed.
  • the battery packaging material of the present invention is used in a package for sealing and housing battery elements such as a positive electrode, a negative electrode, and an electrolyte. That is, a battery element including at least a positive electrode, a negative electrode, and an electrolyte can be accommodated in a package formed of the battery packaging material of the present invention to obtain a battery.
  • a battery element including at least a positive electrode, a negative electrode, and an electrolyte is protruded outside the metal terminal connected to each of the positive electrode and the negative electrode with the battery packaging material of the present invention.
  • a flange portion region where the heat-fusible resin layers contact each other
  • a battery using the battery packaging material is provided.
  • the battery packaging material of the present invention may be used for either a primary battery or a secondary battery, but is preferably a secondary battery.
  • the type of secondary battery to which the battery packaging material of the present invention is applied is not particularly limited.
  • a lithium ion battery, a lithium ion polymer battery, a lead storage battery, a nickel-hydrogen storage battery, a nickel-cadmium storage battery, a nickel- Examples include iron storage batteries, nickel / zinc storage batteries, silver oxide / zinc storage batteries, metal-air batteries, multivalent cation batteries, capacitors, capacitors, and the like.
  • lithium ion batteries and lithium ion polymer batteries are suitable applications for the battery packaging material of the present invention.
  • the battery packaging material according to the first aspect of the present invention effectively suppresses the crushing of the adhesive layer when the heat-fusible resin layers are heat-sealed to each other, and exhibits high sealing strength in a high-temperature environment. To do.
  • the battery packaging material according to the first aspect of the present invention is particularly suitable as a battery packaging material used for a vehicle battery or a mobile device battery that requires high sealing performance of the battery element in a high temperature environment. Can be used.
  • the battery packaging material according to the second aspect of the present invention includes a heat-fusible resin layer in a state where the electrolyte solution is in contact with the heat-fusible resin layer in a high-temperature environment and the electrolyte solution is attached to the heat-fusible resin layer. Even when they are heat-sealed, high sealing strength is exhibited by heat-sealing. For this reason, the battery packaging material according to the second aspect of the present invention can be particularly suitably used as a battery packaging material used in a vehicle battery or a mobile device battery in which an aging process is performed in a high temperature environment. .
  • the battery packaging material according to the third aspect of the present invention suppresses contamination of the mold at the time of molding and exhibits high sealing strength due to heat fusion.
  • the battery packaging material of the third aspect of the present invention is a battery used for a large battery such as a vehicle battery or a stationary battery, in which contamination of the mold due to the lubricant is likely to be a problem and high sealing strength is required. It can be particularly suitably used as a packaging material.
  • Example 1A-3A and Comparative Example 1A-3A As a base material layer, a polyethylene terephthalate (PET) film (thickness 12 ⁇ m) and a stretched nylon (ONy) film (thickness 15 ⁇ m) are prepared, and a two-component urethane adhesive (polyol compound and aromatic isocyanate compound) is applied to the PET film. ) was applied (3 ⁇ m) and adhered to the ONy film.
  • an aluminum alloy foil JIS H4160: 1994 A8021H-O (thickness 40 ⁇ m) was prepared as a barrier layer.
  • a two-component urethane adhesive (polyol compound and aromatic isocyanate compound) was applied to one surface of the aluminum alloy foil to form an adhesive layer (thickness 3 ⁇ m) on the barrier layer.
  • an aging treatment is performed to produce a base material layer / adhesive layer / barrier layer laminate.
  • Chemical conversion treatment is performed on both surfaces of the aluminum alloy foil.
  • the chemical conversion treatment of the aluminum alloy foil is performed on both sides of the aluminum foil by a roll coating method so that the treatment amount of the phenol resin, the chromium fluoride compound, and phosphoric acid is 10 mg / m 2 (dry mass). It was performed by applying and baking.
  • Examples 1A-3A and Comparative Examples 1A-3A the maleic anhydride-modified polypropylene used in the adhesive layer was different, and the logarithmic decay rate ⁇ E (rigid pendulum type physical property test at 120 ° C. shown in Table 1A was used. Value measured using a container).
  • ⁇ Measurement of logarithmic decay rate ⁇ E of adhesive layer> Each of the battery packaging materials obtained above was cut into a rectangle of width (TD: Transverse Direction) 15 mm ⁇ length (MD: Machine Direction) 150 mm to obtain a test sample (battery packaging material 10).
  • the MD of the battery packaging material corresponds to the rolling direction (RD) of the aluminum alloy foil
  • the TD of the battery packaging material corresponds to the TD of the aluminum alloy foil
  • the rolling direction of the aluminum alloy foil (RD) ) Can be identified by the rolling line.
  • MD of the battery packaging material cannot be specified by the rolling line of the aluminum alloy foil, it can be specified by the following method.
  • the cross section of the heat-fusible resin layer of the battery packaging material is observed with an electron microscope to confirm the sea-island structure, and in the direction perpendicular to the thickness direction of the heat-fusible resin layer.
  • the direction parallel to the cross section where the average of the diameter of the island shape is the maximum can be determined as MD.
  • the angle is changed by 10 degrees from the cross section in the length direction of the heat-fusible resin layer and the direction parallel to the cross section in the length direction, and each of the directions up to the direction perpendicular to the cross section in the length direction is changed.
  • the cross section (total of 10 cross sections) is observed with an electron micrograph to confirm the sea-island structure.
  • a diameter y is defined as a linear distance connecting the leftmost end in the vertical direction and the rightmost end in the vertical direction with respect to the thickness direction of the heat-fusible resin layer.
  • the average of the top 20 diameters y is calculated in descending order of the diameter y of the island shape.
  • the direction parallel to the cross section where the average of the diameter y of the island shape is the largest is determined as MD.
  • FIG. 7 shows a schematic diagram for explaining a method of measuring the logarithmic attenuation rate ⁇ E by the rigid pendulum measurement.
  • the frame of the pendulum 30 is FRB-100
  • the edge of the cylindrical cylinder edge 30a is RBP-060
  • the block 31 uses CHB-100
  • a vibration displacement detector 32 and a weight 33
  • the initial amplitude is set to 0.3 degree.
  • the test sample measurement surface is placed on the cooling block 31 so that the axial direction of the cylindrical cylinder edge 30a with the pendulum 30 is perpendicular to the MD direction of the test sample. installed.
  • a tape was attached to a location that does not affect the measurement result of the test sample and fixed on the cooling / heating block 31.
  • a cylindrical cylinder edge was brought into contact with the surface of the adhesive layer.
  • the logarithmic decay rate ⁇ E of the adhesive layer was measured in the temperature range of 30 ° C. to 200 ° C. at a temperature increase rate of 3 ° C./min using the cooling block 31.
  • the logarithmic decay rate ⁇ E in a state where the surface temperature of the adhesive layer of the test sample (battery packaging material 10) was 120 ° C. was adopted.
  • Each battery packaging material obtained above was cut into a length of 150 mm and a width of 60 mm to produce a test sample (battery packaging material 10).
  • the heat-fusible resin layers of the same size test samples prepared from the same battery packaging material were made to face each other.
  • heating and heating were performed in the stacking direction from both sides of the test sample at a temperature of 190 ° C. and each surface pressure (MPa) described in Table 1A for 3 seconds.
  • the heat-fusible resin layers were heat-sealed.
  • the heat-sealed portion of the test sample was cut in the stacking direction using a microtome, and the thickness of the adhesive layer was measured for the exposed cross section.
  • the test sample before heat-sealing was cut in the stacking direction using a microtome, and the thickness of the adhesive layer was measured for the exposed cross section.
  • the ratio of the thickness of the adhesive layer after heat fusion to the thickness of the adhesive layer before heat fusion was calculated, and the remaining ratio (%) of the thickness of the adhesive layer was measured. The results are shown in Table 1A.
  • Each of the battery packaging materials obtained above was cut into a rectangle having a width of 60 mm and a length of 150 mm to obtain a test sample (battery packaging material 10).
  • the test sample was folded at the center P in the length direction, and the heat-fusible resin layers were opposed to each other.
  • the surface pressure is 1.0 MPa
  • the time is 1 second
  • the temperature is 190 ° C.
  • the test sample is 7 mm (the width of the metal plate) in the length direction and the entire width direction (ie, 60 mm).
  • the heat-fusible resin layers were heat-fused.
  • the test sample was cut to a width of 15 mm as shown in FIG. In FIG. 5, the heat-sealed region is indicated by S.
  • FIG. 6 using a tensile tester so as to be T-shaped peeling, in an environment at a temperature of 25 ° C. or an environment at a temperature of 140 ° C., a tensile speed of 300 mm / min, a peeling angle of 180 °, When the distance between chucks is 50 mm, the thermally fused interface is peeled off, and the maximum peel strength (N / 15 mm) for 1.5 seconds from the start of tensile strength measurement is the seal strength in a 25 ° C environment.
  • the sealing strength was 140 ° C.
  • the tensile test at each temperature was performed in a thermostat, and the test sample was attached to the chuck and held for 2 minutes in the thermostat at a predetermined temperature, and measurement was started.
  • the battery packaging materials of Examples 1A to 3A are logarithmic at 120 ° C. in the rigid pendulum measurement of the adhesive layer located between the barrier layer and the heat-fusible resin layer. It can be seen that the attenuation factor ⁇ E is 2.0 or less, the collapse of the adhesive layer when the heat-fusible resin layers are heat-sealed is effectively suppressed, and high sealing strength is exhibited in a high-temperature environment. .
  • Example 1B and Comparative Example 1B As a base material layer, a polyethylene terephthalate (PET) film (thickness 12 ⁇ m) and a stretched nylon (ONy) film (thickness 15 ⁇ m) are prepared, and a two-component urethane adhesive (polyol compound and aromatic isocyanate compound) is applied to the PET film. ) was applied (3 ⁇ m) and adhered to the ONy film. Moreover, an aluminum foil (JIS H4160: 1994 A8021H-O (thickness 40 ⁇ m)) was prepared as a barrier layer.
  • PTT polyethylene terephthalate
  • ONy stretched nylon
  • urethane adhesive polyol compound and aromatic isocyanate compound
  • a two-component urethane adhesive (a polyol compound and an aromatic isocyanate compound) was applied to one surface of the aluminum foil to form an adhesive layer (thickness 3 ⁇ m) on the barrier layer.
  • an aging treatment is performed to produce a base material layer / adhesive layer / barrier layer laminate. did.
  • Chemical conversion treatment is performed on both surfaces of the aluminum foil.
  • the chemical conversion treatment of the aluminum foil is performed on both surfaces of the aluminum foil by a roll coating method so that the coating amount of chromium is 10 mg / m 2 (dry mass) with a treatment solution comprising a phenol resin, a chromium fluoride compound, and phosphoric acid. This was done by applying and baking.
  • an acid-modified polypropylene as an adhesive layer (thickness 40 ⁇ m) and a polypropylene as a heat-fusible resin layer (thickness 40 ⁇ m) are coextruded on the barrier layer of each laminate obtained above.
  • the heat-fusible resin layer is measured by the method described later by adjusting the amount of the low molecular weight component in polypropylene, and the starting point of the melting peak temperature of the heat-fusible resin layer (extrapolated melting start temperature). And a value (T 2 / T 1 ) obtained by dividing the temperature difference T 2 between the end point and the end point (extrapolation end temperature) by the temperature difference T 1 is adjusted.
  • the polypropylene used for the heat-fusible resin layer has a lithium hexafluorophosphate concentration of 1 mol / l and a volume ratio of ethylene carbonate, diethyl carbonate and dimethyl carbonate of 1: 1: After leaving still for 72 hours in the electrolyte solution which is the solution of 1, it was made to fully dry. Next, a DSC curve was obtained for the dried polypropylene using differential scanning calorimetry (DSC) in accordance with the provisions of JIS K7121: 2012. Next, from the obtained DSC curve, the temperature difference T 2 between the extrapolation melting start temperature and the extrapolation melting end temperature of the melting peak temperature of the heat-fusible resin layer after drying was measured.
  • DSC differential scanning calorimetry
  • the DSC curve at the time of raising the temperature to 200 ° C. was used for the second time. Also, when measuring the temperature difference T 1 and temperature difference T 2 , analyze the melting peak that maximizes the difference in thermal energy input among the melting peaks that appear in the range of 120 to 160 ° C in each DSC curve. went. Even when two or more peaks were overlapped, only the melting peak where the difference in the input of thermal energy was maximized was analyzed.
  • the extrapolated melting start temperature means the starting point of the melting peak temperature, and the melting that maximizes the difference between the heat energy input and the straight line obtained by extending the base line on the low temperature (65 to 75 ° C) side to the high temperature side.
  • the temperature at the intersection of the tangent drawn on the curve on the low temperature side of the peak at the point where the gradient is maximum is used.
  • Extrapolation end temperature means the end of the melting peak temperature, and the high temperature side of the melting peak where the difference between the heat energy input and the straight line obtained by extending the base line on the high temperature (170 ° C) side to the low temperature side becomes the maximum.
  • the temperature at the point of intersection with the tangent drawn on the curve at the point where the gradient is maximum is taken.
  • ⁇ Measurement of seal strength before electrolyte contact> tensile strength (seal strength) was measured in the same manner except that the electrolyte solution was not injected into the test sample. The maximum tensile strength until the heat-sealed portion is completely peeled is defined as the seal strength before contact with the electrolyte.
  • the seal strength before contact with the electrolyte is described as the seal strength when the contact time of the electrolyte at 85 ° C. is 0 h.
  • each of the battery packaging materials obtained above was cut into a rectangle of width (x direction) 100 mm ⁇ length (z direction) 200 mm to obtain a test sample (battery packaging material 10 (FIG. 9a).
  • the test sample (battery packaging material 10) was folded at the center in the z direction so that the heat-fusible resin layer side overlapped (FIG. 9b).
  • both ends in the x direction of the folded test sample were sealed with a heat seal (temperature 190 ° C., surface pressure 2.0 MPa, time 3 seconds), and formed into a bag shape having one opening E (FIG. 9c).
  • an electrolytic solution concentration of lithium hexafluorophosphate is 1 mol / l and the volume ratio of ethylene carbonate, diethyl carbonate, and dimethyl carbonate is 1: 1: from the opening E of the test sample formed into a bag shape. 6g (FIG. 9d), and the end of the opening E was sealed by heat sealing (temperature 190 ° C., surface pressure 2.0 MPa, time 3 seconds) (FIG. 9e).
  • the folded portion of the bag-shaped test sample was placed downward, and was allowed to stand for a predetermined storage time (72 hours, 120 hours, etc., which is a time for contact with the electrolytic solution) in an environment at a temperature of 85 ° C.
  • the end portion of the test sample was cut (FIG. 9e), and all the electrolyte solution was discharged.
  • the electrolytic solution adhering to the surface of the heat-fusible resin layer, the upper and lower surfaces of the test sample are sandwiched between the metal plates 20 (7 mm width), the temperature is 190 ° C., the surface pressure is 1.0 MPa, and the time is 3 seconds.
  • the heat-fusible resin layers were heat-fused under the conditions (FIG. 9f).
  • the test sample was cut to a width of 15 mm with a double-edged sample cutter so that the seal strength at a width (x direction) of 15 mm could be measured (FIGS. 9f, g).
  • Table 2B shows the retention ratio (%) of the seal strength after contact with the electrolyte, based on the seal strength before contact with the electrolyte (100%).
  • the battery packaging material of Example 1B has a value obtained by dividing the temperature difference T 2 by the temperature difference T 1 of 0.60 or more, and is heat-fusible in a high temperature environment. Even when the heat-fusible resin layers are heat-sealed with the electrolyte layer in contact with the resin layer and the electrolyte solution is attached to the heat-fusible resin layer, high sealing strength is exhibited by heat-sealing. I understand that.
  • Example 1C-3C and Comparative Example 1C-2C As a base material layer, a polyethylene terephthalate (PET) film (thickness 12 ⁇ m) and a stretched nylon (ONy) film (thickness 15 ⁇ m) are prepared, and a two-component urethane adhesive (polyol compound and aromatic isocyanate compound) is applied to the PET film. ) was applied (3 ⁇ m) and adhered to the ONy film.
  • an aluminum alloy foil JIS H4160: 1994 A8021H-O (thickness 40 ⁇ m) was prepared as a barrier layer.
  • a two-component urethane adhesive (polyol compound and aromatic isocyanate compound) was applied to one surface of the aluminum alloy foil to form an adhesive layer (thickness 3 ⁇ m) on the barrier layer.
  • an aging treatment is performed to produce a base material layer / adhesive layer / barrier layer laminate.
  • Chemical conversion treatment is performed on both surfaces of the aluminum alloy foil.
  • the chemical conversion treatment of the aluminum alloy foil is performed on both sides of the aluminum foil by a roll coating method so that the treatment amount of the phenol resin, the chromium fluoride compound, and phosphoric acid is 10 mg / m 2 (dry mass). It was performed by applying and baking.
  • an acid-modified polyolefin as an adhesive layer (thickness 40 ⁇ m) and polypropylene as a heat-fusible resin layer (thickness 40 ⁇ m) are coextruded on the barrier layer of each laminate obtained above.
  • the tensile modulus measured by the method described later is adjusted by adjusting the molecular weight of the resin constituting the heat-fusible resin layer, the melt mass flow rate (MFR), and the like.
  • the base material layer and the heat-fusible resin layer were mixed with a predetermined amount (700 ppm) of erucic acid amide as a lubricant. Specifically, erucic acid amide was blended in the resin constituting the base material layer and the heat-fusible resin layer, and erucic acid amide was bleed out on the surface of the base material layer and the heat-fusible resin layer.
  • each battery packaging material was cut to prepare a test sample (battery packaging material 10) of 80 mm (TD: Transverse Direction) ⁇ 200 mm (MD: Machine Direction).
  • TD Transverse Direction
  • MD Machine Direction
  • the test sample is allowed to stand on the surface of the rectangular metal plate 11 placed on the horizontal surface 21 so that the heat-fusible resin layer 4 side faces downward.
  • a weight 12 having a weight of 200 g is placed on the surface of the test sample on the base material layer side.
  • the metal plate 11 has a surface Rz (maximum height roughness) of 0.8 ⁇ m as defined in Table 2 of Comparative Surface Roughness Standard Strip for JIS B 0659-1: 2002 Annex 1 (reference). Made of stainless steel. Moreover, the area which the surface of the metal plate 11 and the heat-fusible resin layer 4 of a test sample contact is 160 cm ⁇ 2 > (the surface which is contacting is square). Moreover, the area which the weight 12 and the surface by the side of the base material layer of a test sample contact is 40 cm ⁇ 2 > (the surface which is contacting is square). The dynamic friction coefficient was calculated by dividing the obtained dynamic friction force (N) by the normal force of the weight (1.96 N). The results are shown in Table 1C.
  • Each of the battery packaging materials obtained above was cut into a rectangle having a width of 60 mm and a length of 150 mm to obtain a test sample (battery packaging material 10). As shown in FIG. 6, the test sample was folded at the center P in the length direction, and the heat-fusible resin layers were opposed to each other. Next, using a metal plate 20 having a width of 7 mm, under the conditions of a temperature of 190 ° C., a surface pressure of 1.0 MPa, and a time of 1 second, the length of the test sample is 7 mm (the width of the metal plate) and the entire width direction (ie, 60 mm). ), The heat-fusible resin layers were heat-fused.
  • the test sample was cut so as to have a width of 15 mm. 5 and 6, the heat-sealed region is indicated by S.
  • the heat-sealed region is indicated by S.
  • a tensile tester manufactured by Shimadzu Corp., AGS-xplus (trade name)
  • the tensile strength was measured by peeling off the heat-sealed interface under the conditions of a tensile speed of 300 mm / min, a peeling angle of 180 °, and a distance between chucks of 50 mm.
  • Seal strength after 1 second from the start of measurement (N / 15mm), seal strength after 2.5 seconds from the start of measurement (N / 15mm), and seal strength after 10 seconds from the start of measurement (N / 15mm) Is shown in Table 1C.
  • the value of each seal strength is an average value measured for three test samples.
  • Rz maximum height roughness made of stainless steel with a surface of 0.8 ⁇ m, corner R3.5) and a corresponding molding die (male, JIS B0659-1: 2002 attachment) 1 (for reference), using a surface roughness standard piece for comparison, specified in Table 2 and made of stainless steel having a surface with a surface roughness Rz (maximum height roughness) of 0.8 ⁇ m, corner R3.0).
  • Cold forming one-step drawing was performed 500 times continuously at a forming depth of 5.0 mm at a pressure (surface pressure) of 0.2 MPa.
  • the male mold was placed on the heat-fusible resin layer side of the test sample and molded. The clearance between the male mold and the female mold is 0.5 mm.
  • the tensile modulus of the heat-fusible resin layer measured in accordance with JIS K7161: 2014 is in the range of 500 to 1000 MPa.
  • the battery packaging material has a seal strength of 100 N / 15 mm or more from the start of measurement to the end of 2.5 seconds, and further to the end of 10 seconds, and has an excellent seal strength. It was.
  • mold contamination was suppressed, and both high sealing strength and mold contamination suppression were compatible.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Mechanical Engineering (AREA)
  • Sealing Battery Cases Or Jackets (AREA)
  • Laminated Bodies (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)
PCT/JP2018/016359 2017-04-20 2018-04-20 電池用包装材料、その製造方法、及び電池 Ceased WO2018194171A1 (ja)

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EP18787250.2A EP3614449B1 (en) 2017-04-20 2018-04-20 Battery packaging material, method for manufacturing the same, and battery
KR1020247030619A KR20240144420A (ko) 2017-04-20 2018-04-20 전지용 포장 재료, 그의 제조 방법 및 전지
KR1020197027134A KR102308638B1 (ko) 2017-04-20 2018-04-20 전지용 포장 재료, 그의 제조 방법 및 전지
KR1020227023290A KR20220101016A (ko) 2017-04-20 2018-04-20 전지용 포장 재료, 그의 제조 방법 및 전지
JP2018553495A JP6465261B1 (ja) 2017-04-20 2018-04-20 電池用包装材料、その製造方法、及び電池
CN201880003134.5A CN109564995B (zh) 2017-04-20 2018-04-20 电池用包装材料、其制造方法和电池
US16/604,895 US20200194737A1 (en) 2017-04-20 2018-04-20 Battery packaging material, method for producing the same, and battery
KR1020217031018A KR102419865B1 (ko) 2017-04-20 2018-04-20 전지용 포장 재료, 그의 제조 방법 및 전지
EP24190388.9A EP4428996A3 (en) 2017-04-20 2018-04-20 Battery packaging material, method for manufacturing the same, and battery
US18/230,894 US20230387519A1 (en) 2017-04-20 2023-08-07 Battery packaging material, method for producing the same, and battery

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JP7694416B2 (ja) 2020-06-12 2025-06-18 大日本印刷株式会社 蓄電デバイス用外装材、その製造方法、及び蓄電デバイス
WO2021251501A1 (ja) * 2020-06-12 2021-12-16 大日本印刷株式会社 蓄電デバイス用外装材、その製造方法、及び蓄電デバイス
US12542317B2 (en) 2020-06-12 2026-02-03 Dai Nippon Printing Co., Ltd. Exterior material for power storage device, method for manufacturing same, and power storage device
WO2022234790A1 (ja) * 2021-05-06 2022-11-10 昭和電工パッケージング株式会社 ラミネート外装材
JPWO2022234790A1 (https=) * 2021-05-06 2022-11-10
KR20240100236A (ko) * 2022-12-22 2024-07-01 주식회사 엘지에너지솔루션 파우치 필름 적층체 및 이차 전지
KR102876483B1 (ko) * 2022-12-22 2025-10-28 주식회사 엘지에너지솔루션 파우치 필름 적층체 및 이차 전지

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