The present disclosure relates to a terminal coating resin film used for sealing current output terminals of a power storage device or a power generation device, and a power storage device using the terminal coating resin film.
In recent years, there is an increasing need of downsized mobile devices and effective usage of electrical energy generated from natural resources. In response to this, research and development of lithium ion batteries (a type of power storage devices) providing higher voltage and having higher energy density are underway. As packaging materials used for such lithium ion batteries, metal cans have typically been used. Recently, to meet the need for providing thinner and more diversified products to which the lithium ion batteries are applied, pouched laminates configured by a metal layer (e.g., aluminum foil) and a resin film, which can be produced at low cost, have become mainstream as packaging materials.
A lithium ion battery in which a battery body is sealed in the above packaging material is referred to as a laminated lithium ion battery. This type of lithium ion battery is provided with current output terminals (which may also be referred to as tab leads). For purposes such as improving adhesion between each current output terminal and the packaging material, a terminal coating resin film (which may also be referred to as a tab sealant) may be arranged covering part of the outer periphery of the current output terminal (e.g., see PTLs 1 to 3).
Power storage devices, which are referred to as fully solid-state batteries, are under research and development as next generation batteries replacing lithium ion batteries. Fully solid-state batteries are characterized by usage of a solid electrolyte as an electrolytic substance, without using an organic electrolyte solution. Lithium ion batteries cannot be used under temperature conditions higher than the boiling point of their electrolyte solution (about 80° C.), whereas fully solid-state batteries can be used under temperature conditions higher than 100° C., and can enhance conductivity of the lithium ions when the batteries are used under high temperature conditions (e.g., 100° C. to 150° C.).
However, if laminated fully solid-state batteries are produced using the laminates mentioned above as packaging materials, sealing properties of the packages for the fully solid-state batteries may be insufficient due to the terminal coating resin films having insufficient heat resistance.
The present disclosure has been made in light of the issues set forth above and aims to provide a terminal coating resin film having good heat resistance, and a power storage device using the terminal coating resin film.
A terminal coating resin film according to the present disclosure is characterized in that it is used for sealing a current output terminal in at least one of a power storage device and a power generation device. The terminal coating resin film comprises a resin composition having adhesion to the current output terminal. The resin composition contains at least one of a thermosetting resin and a thermoplastic resin having a melting point of 160° C. or higher, and does not contain any thermoplastic resin having a melting point of less than 160° C.
Terminal coating resin films of conventional art mainly comprise polypropylene, and have a melting point of about 150° C. Therefore, the heat resistance of conventional terminal coating resin films is insufficient if the films are used, for example, in fully solid-state batteries that can have a temperature in the range of 100° C. to 150° C. In this regard, the terminal coating resin film according to the present disclosure has good heat resistance because it contains at least one of a thermosetting resin and a thermoplastic resin having a melting point of 160° C. or higher, and does not contain any thermoplastic resin having a melting point of less than 160° C. Accordingly, if a power storage device or a power generation device is used under temperature conditions, for example, in the range of 100° C. to 150° C., sealing properties of the packages of these devices can be sufficiently maintained. Furthermore, if high current is passed through the current output terminal of the power storage device or the power generation device and the temperature of the current output terminal reaches a temperature range, for example, of 100° C. to 150° C., sealing properties of the packages of these devices can be sufficiently maintained. The melting point herein refers to a peak melting temperature which is calculated according to the method described in JIS K7121-1987. If there are two or more independent melting peaks, the lowest peak melting temperature is used.
Power storage devices to which the terminal coating resin film of the present disclosure can be applied may be fully solid-state batteries. However, without being limited to this, the terminal coating resin film may be applied to other power storage devices or power generation devices.
In the present disclosure, the thermosetting resin may be at least one selected from the group consisting of polyimide resins, phenol resins, urea resins, melamine resins, unsaturated polyester resins, urethane resins, allyl resins, epoxy resins, furan resins, and silicone resins. These thermosetting resins have good adhesion to the metal material (e.g., aluminum or nickel) configuring the surface of the current output terminal, and have good heat resistance.
In the present disclosure, the thermoplastic resin may be at least one selected from the group consisting of polyester resins (e.g., polyethylene terephthalate (PET) and copolymers thereof, and polyester resins based on PET components), nylons, polyvinyl alcohol resins, polyvinylidene chloride, polyamide resins, polybutylene terephthalate resins, polyphenylene sulfide, polyetherimide, polysulfone, fluororesins, polyamide imide, and acetyl cellulose. These thermoplastic resins have good adhesion to the metal material (e.g., aluminum or nickel) configuring the surface of the current output terminal, and have good heat resistance.
The terminal coating resin film according to the present disclosure may have a single layer structure or a multilayer structure. If the terminal coating resin film has a single layer structure, the resin composition forming the terminal coating resin film is preferred to be one selected from the group consisting of polyester resins, polyphenylene sulfide, urethane resins, and epoxy resins. Use of a film comprising these resins as a terminal coating resin film can easily achieve an advantageous effect of adhesion to the current output terminal (appropriate fluidity of the resin composition during heat sealing), balanced with insulation properties of the current output terminal (prevention of excessive fluidity of the resin composition during heat sealing).
If the terminal coating resin film has a multilayer structure, the terminal coating resin film can include a first layer and a second layer. The first layer may comprise a resin which is selected from the group consisting of polyester resins having a melting point in the range of 170° C. to 280° C. and polyphenylene sulfide (PPS) having a melting point in the range of 260° C. to 290° C. The second layer may comprise either a thermosetting resin or a thermoplastic resin having a melting point in the range of 160° C. to 280° C. The second layer is preferred to be formed on a surface of the first layer facing the current output terminal. If PET or PPS having a sufficiently high melting point is used as a resin for forming the first layer, the first layer will not melt at the time of heat sealing and thus good insulation properties may be achieved for the current output terminal.
If the terminal coating resin film has a multilayer structure including the first and second layers, the terminal coating resin film may further include a third layer formed on a surface of the first layer facing away from the surface on which the second layer is formed. The third layer may comprise a thermosetting resin or a thermoplastic resin having a melting point in the range of 160° C. to 280° C.
If the terminal coating resin film has a multilayer structure, the first layer may comprise a thermosetting resin. In this case, the terminal coating resin film is preferred to include a thermosetting resin layer formed at least on one surface of the first layer, and the thermosetting resin layer is preferred to have fluidity which is higher than that of the thermosetting resin forming the first layer. Use of such a configuration can achieve good adhesion to the current output terminal.
The present disclosure provides a power storage device (e.g., fully-solid state battery) including a power storage device body, a current output terminal extended from the power storage device body, a packaging material sandwiching the current output terminal between surfaces thereof and holding the power storage device body therein, and the terminal coating resin film set forth above disposed between the current output terminal and the packaging material.
According to the present disclosure, a terminal coating resin film having good heat resistance, and a power storage device using the terminal coating resin film can be provided.
Embodiments of the present invention of will be described below with reference to the drawings. In the following description of the drawings to be referred, components or functions identical with or similar to each other are given the same or similar reference signs, unless there is a reason not to. It should be noted that the drawings are only schematically illustrated, and thus the relationship between thickness and two-dimensional size of the components, and the thickness ratio between the layers, are not to scale. Therefore, specific thicknesses and dimensions should be understood in view of the following description. As a matter of course, dimensional relationships or ratios may be different between the drawings.
Further, the embodiments described below are merely examples of configurations for embodying the technical idea of the present invention. The technical idea of the present invention does not limit the materials, shapes, structures, arrangements, and the like of the components to those described below. The technical idea of the present invention can be modified variously within the technical scope defined by the claims. The present invention is not limited to the following embodiments within the scope not departing from the spirit of the present invention.
<Power Storage Device>
The power storage device 100 as a fully solid-state battery includes a power storage device body 10, a packaging material 20, two metal terminals 30 (current output terminals), and a terminal coating resin film 40 (tab sealant). The power storage device body 10 is a battery body that charges or discharges current. The packaging material 20 is arranged covering surfaces of the power storage device body 10 and in contact with part of the terminal coating resin film 40.
(Packaging Material)
The inner layer 18 contains polyethylene terephthalate (PET) and/or a copolymer thereof and has a peak melting temperature in the range of 160° C. to 280° C. The substrate layer 11 is preferred to have a peak melting temperature higher than that of the inner layer 18. If the substrate layer 11 has a peak melting temperature higher than that of the inner layer 18, the appearance of the packaging material 20 is prevented from being impaired due to melting of the substrate layer 11 (outer layer) at the time of heat sealing. First, the inner layer 18 and the substrate layer 11 will be explained as follows.
As the inner layer 18, a commercially available crystalline PET film (peak melting temperature: about 255° C.) may be used. The peak melting temperature of the inner layer 18 may be controlled according to the heat resistance required of the inner layer 18 (e.g., activation temperature conditions of the power storage device 100). For example, a crystallinity-controlled or unstretched crystalline PET film, or a copolymer film containing units of polyethylene terephthalate and units of another resin, or a PET film containing crystalline PET and amorphous PET may be used. Alternatively, a polyester resin which is based on PET components may be used as a material for the inner layer 18. Such a polyester resin has structural units derived from ethylene glycol, structural units derived from a terephthalic acid, and other structural units. Dihydric alcohol components from which the structural units of the polyester resin are derived may include neopentyl glycol, 1,4-butanediol, and diethylene glycol. Acid components from which the structural units of the polyester resin is derived may include an isophthalic acid, adipic acid, and sebacic acid. The melting point of the polyester resin can be controlled by controlling the amount of these structural units. In the following, a copolymer of PET or a polyester resin based on a component of PET is termed a PET resin.
As mentioned above, the peak melting temperature of the inner layer 18 may be in the range of 160° C. to 280° C. If the temperature is less than 160° C., heat resistance of the inner layer 18 may be insufficient, and if it exceeds 280° C., the temperature for heat sealing may be excessively high. The lower limit of the peak melting temperature of the inner layer 18 may be 165° C., 175° C., 185° C., 195° C., 200° C., 205° C., 215° C., 225° C. or 235° C. The upper limit of the peak melting temperature of the inner layer 18 may be 275° C., 268° C., 262° C. or 252° C.
The inner layer 18 may have a single layer structure, or may have a multilayer structure. As shown in
The inner layer 18, if it has a single layer structure, is preferred to have a thickness in the range of 10 μm to 100 μm and more preferably 20 μm to 80 μm. When the inner layer 18 has a thickness of 10 μm or more, sealing properties and insulation properties may be easily secured, and when it has a thickness of 100 μm or less, the production cost may be reduced.
As shown in
The first layer 18a is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the first layer 18a has a thickness of 5 μm or more, insulation properties can be easily secured, and when it has a thickness of 500 μm or less, the production cost can be reduced.
From the perspectives of heat resistance and sealing strength, the second layer 18b may contain a thermosetting resin instead of PET and/or PET resin, or may contain both PET and/or PET resin and a thermosetting resin. The thermosetting resin may be a polyimide resin, phenol resin, urea resin, melamine resin, unsaturated polyester resin, urethane resin, allyl resin, epoxy resin, furan resin, or silicone resin. These resins may be used singly or in combination of two or more.
The second layer 18b is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the second layer 18b has a thickness of 5 μm or more, sealing properties can be easily secured, and when it has a thickness of 500 μm or less, the production cost can be reduced.
As shown in
From the perspectives of heat resistance and sealing strength, the third layer 18c may contain a thermosetting resin instead of PET and/or PET resin, or may contain both PET and/or PET resin and a thermosetting resin. The thermosetting resin may be a polyimide resin, phenol resin, urea resin, melamine resin, unsaturated polyester resin, urethane resin, allyl resin, epoxy resin, furan resin, or silicone resin. These resins may be used singly or in combination of two or more.
The third layer 18c is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the third layer 18c has a thickness of 5 μm or more, high sealing strength can be easily secured, and when it has a thickness of 500 μm or less, the production cost can be reduced. The second and third layers 18b and 18c may have the same configuration or different configurations. The inner layer 18 may contain, for example, various additives (e.g., a flame retarder, slip agent, anti-blocking agent, antioxidant, light stabilizer, and tackifier).
As mentioned above, the substrate layer 11 may have a peak melting temperature higher than that of the inner layer 18. If the inner layer 18 has a multilayer structure, the peak melting temperature of the inner layer 18 refers to that of the layer (e.g., the first layer 18a) having a maximum peak melting temperature. The substrate layer 11 is preferred to have a peak melting temperature higher than that of the inner layer 18 by 10° C. or more, and preferably 30° C. or more. The resin film that can be used for the substrate layer 11 and has a peak melting temperature in the above range may be a nylon film, PET film, polyamide film, polyphenylene sulfide film (PPS film), or the like. The substrate layer 11 may be a commercially available film, or may be a coating film (obtained by applying and drying a coating liquid). The substrate layer 11 may have a single layer structure or a multilayer structure, or may be formed by applying a thermosetting resin. The substrate layer 11 may contain, for example, various additives (e.g., a flame retarder, slip agent, anti-blocking agent, antioxidant, light stabilizer, and tackifier).
When the peak melting temperature of the substrate layer 11 is expressed as T11 and that of the inner layer 18 is expressed as T18, the difference therebetween (T11-T18) is preferred to be 20° C. or more, and more preferably in the range of 40° C. to 100° C. When the temperature difference is 20° C. or more, the appearance of the packaging material 20 is even more sufficiently prevented from being impaired due to heat sealing. The substrate layer 11 is preferred to have a thickness in the range of 5 μm to 50 μm, and more preferably 12 μm to 30 μm.
The following description explains the first adhesive layer 12a, the first anticorrosion treatment layer 13a, the barrier layer (metal foil layer) 15, the second anticorrosion treatment layer 13b, and the second adhesive layer 12b. These layers have heat resistance equivalent to or exceeding that of the inner layer 18 or the substrate layer 11.
The adhesive layers 12a and 12b may have sufficient heat resistance. Thus, a known adhesive can be appropriately selected and used, such as a generally used adhesive for dry lamination, an acid-modified thermally adhesive resin, thermosetting adhesive, or the like. The thermosetting adhesive may, for example, be a polyester urethane adhesive, or epoxy adhesive.
The barrier layer 15 is a metal layer having electrical conductivity. The material used for the barrier layer 15 may, for example, be aluminum, stainless steel, or the like. However, from the perspective of cost or weight (density), aluminum is preferred. The anticorrosion treatment layers 13a and 13b protect the barrier layer 15. As an example of the anticorrosion treatment layers 13a and 13b, those layers which contain a rare earth element oxide (e.g., cerium oxide), and phosphoric acid or phosphate may be mentioned. As shown in
(Metal Terminal)
Metal can be used as a material for the metal terminals 30. The material used for the metal terminals 30 may be determined considering, for example, the structure of the power storage device body 10, materials of the components of the power storage device body 10, and the like. For example, if the power storage device 100 is a fully solid-state battery, aluminum is preferred to be used as a material for the metal terminal 30 connected to the positive electrode of the power storage device body 10. As a material for the metal terminal 30 connected to the negative terminal of the power storage device body 10, copper having a nickel-plated layer on the surface thereof, or nickel is preferred to be used.
The metal terminals 30 each have a thickness depending on the size or capacity of the fully solid-state battery. If the fully solid-state battery has a small size, the thickness of each metal terminal 30 may be 50 μm or more, for example. If the fully solid-state battery has a large size suitable for electrical storage or vehicle installation, the thickness of each metal terminal 30 can be appropriately determined within the range of 100 μm to 500 μm, for example.
(Terminal Coating Resin Film)
As shown in
The terminal coating resin film 40 comprises a resin composition having adhesion to the metal terminal 30. The resin composition contains at least one of a thermosetting resin and a thermoplastic resin having a peak melting temperature (melting point) of 160° C. or higher, and does not contain any thermoplastic resin having a peak melting temperature of less than 160° C. The terminal coating resin film 40 having such a configuration can sufficiently maintain sealing properties of the power storage device 100 even when the power storage device is used under temperature conditions in the range of 100° C. to 150° C., for example, or even when the temperature of the metal terminal 30 reaches a temperature range of 100° C. to 150° C., for example. The resin composition may contain at least one of a thermosetting resin and a thermoplastic resin having a peak melting temperature (melting point) of 200° C. or higher, and may contain no thermoplastic resin having a peak melting temperature of less than 200° C.
The thermosetting resin used for the terminal coating resin film 40 may be at least one selected from the group consisting of polyimide resins, phenol resins, urea resins, melamine resins, unsaturated polyester resins, urethane resins, allyl resins, epoxy resins, furan resins, and silicone resins. These thermosetting resins have good adhesion to the metal material (e.g., aluminum or nickel) configuring the surface of the metal terminal 30, and good heat resistance.
The thermoplastic resin used for the terminal coating resin film 40 may be at least one selected from the group consisting of PET, the PET resins mentioned above, nylons, polyvinyl alcohol resins, polyvinylidene chloride, polyamide resins, polybutylene terephthalate resins, polyphenylene sulfide, polyetherimide, polysulfone, fluororesins, polyamide imide, and acetyl cellulose. These thermoplastic resins have good adhesion to the metal material (e.g., aluminum or nickel) configuring the surface of the metal terminal 30, and good heat resistance.
The terminal coating resin film 40 may have a single layer structure or a multilayer structure. If the terminal coating resin film 40 has a single layer structure (see
If the terminal coating film 40 has a multilayer structure, the terminal coating resin film 40 may include a first layer 40a and a second layer 40b which is formed on the surface of the first layer 40a facing the metal terminal 30. The first layer 40a in this case comprises PET and/or a PET resin having a peak melting temperature in the range of 170° C. to 270° C., or polyphenylene sulfide (PPS) having a peak melting temperature in the range of 260° C. to 300° C., and the second layer 40b comprises a thermosetting resin, or a thermoplastic resin having a peak melting temperature in the range of 160° C. to 270° C. (see
The first layer 40a is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the first layer 40a has a thickness of 5 μm or more, insulation properties can be easily secured, and if it has a thickness of 500 μm or less, the production cost can be reduced. The second layer 40b is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the second layer 40b has a thickness of 5 μm or more, sealing properties can be easily secured, and if it has a thickness of 500 μm or less, the production cost can be reduced.
If the terminal coating resin film 40 has a multilayer structure including the first and second layers 40a and 40b, the film 40 may further include a third layer 40c which is formed on a surface of the first layer 40a facing away from the surface on which the second layer 40b is formed (see
If the first layer 40a comprises a thermosetting resin, the second layer 40b is preferred to be made of a thermosetting resin whose fluidity is higher than that of the thermosetting resin forming the first layer 40a. With this configuration, good adhesion to the metal terminal 30 can be achieved by the second layer 40b during heat sealing. The third layer 40c may be made of a thermosetting resin whose fluidity is higher than that of the thermosetting resin forming the first layer 40a. With this configuration, a power storage device 100 having even better adhesion can be achieved.
The third layer 40c is preferred to have a thickness in the range of 5 μm to 500 μm, and more preferably 20 μm to 200 μm. When the third layer 40c has a thickness of 5 μm or more, sealing properties can be easily secured, and if it has a thickness of 500 μm or less, the production cost can be reduced.
An embodiment of the present disclosure has been described so far, but the present invention should not be limited to the embodiment described above. In the embodiment described above, a fully solid-state battery has been shown as a power storage device, for example, to which the terminal coating resin film 40 is applied. However, the terminal coating resin film 40 may be applied to other power storage devices (e.g., lithium ion batteries), or power generation devices.
In the following, the present disclosure will be more specifically described by way of examples. However, the present invention should not be limited to the following examples.
<Preparation of Packaging Material>
As a substrate layer, a highly heat resistant polyamide film (thickness: 25 manufactured by Unitika, Ltd.) having a peak melting temperature of 300° C. was used. As a metal foil layer, an aluminum foil (thickness 40 μm) was prepared. As an inner layer, a PET film (thickness: 75 single layer structure) having a peak melting temperature of 255° C. was prepared. The substrate layer and the metal foil layer were bonded to each other using a thermosetting adhesive (polyester urethane adhesive), while the metal foil layer and the inner layer were bonded to each other using the same adhesive to thereby obtain a packaging material having sufficient heat resistance.
<Preparation of Terminal Coating Resin Film (Single Layer Structure)>
An epoxy resin film (thickness: 100 μm) was prepared as a terminal coating resin film (single layer structure).
A urethane resin film (thickness: 100 μm) was prepared as a terminal coating resin film (single layer structure).
A nylon resin film (thickness: 100 μm, melting point: 225° C.) was prepared as a terminal coating resin film (single layer structure).
A PET film (thickness: 100 μm, melting point: 225° C.) was prepared as a terminal coating resin film (single layer structure).
A polyester copolymer film (thickness: 100 μm, melting point: 160° C.) was prepared as a terminal coating resin film (single layer structure).
A PPS film (thickness: 100 μm, melting point: 290° C.) was prepared as a terminal coating resin film (single layer structure).
A PP film (thickness: 100 μm, melting point: 140° C.) was prepared as a terminal coating resin film (single layer structure).
<Preparation of Terminal Coating Resin Film (Two-Layer Structure)>
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: Epoxy resin film (thickness: 50 μm)
Second layer: PET film (thickness: 50 μm, melting point: 255° C.)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: Urethane resin film (thickness: 50 μm)
Second layer: Epoxy resin film (thickness: 50 μm)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: Epoxy resin film (thickness: 50 μm)
Second layer: Epoxy resin film (thickness: 50 μm)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: PPS film (thickness: 50 μm, melting point: 290° C.)
Second layer: PET film (thickness: 50 μm, melting point: 255° C.)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: PPS film (thickness: 50 μm, melting point: 290° C.)
Second layer: Epoxy resin film (thickness: 50 μm)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: Epoxy resin film (thickness: 50 μm)
Second layer: PP film (thickness: 50 melting point 140° C.)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: PP film (thickness: 50 melting point 140° C.)
Second layer: Epoxy resin film (thickness: 50 μm)
A two-layer structure terminal coating resin film including a first layer and a second layer was prepared by bonding the following films to each other.
First layer: PP film (thickness: 50 melting point 140° C.)
Second layer: PET film (thickness: 50 melting point: 255° C.)
<Evaluation of Insulation Properties>
Referring to
A: 200 MΩ or more
B: 30 MΩ or more and less than 200 MΩ
C: Less than 30 MΩ
<Evaluation of Adhesion to Current Output Terminal>
Measurement samples were prepared as in the above item <Evaluation of insulation properties>except that no exposed portion 57 of the metal foil layer was formed. A red penetrant (manufactured by TASETO Co., Ltd.) was sprayed on the joint between the current output terminal and the terminal coating film of each of the samples of examples and comparative examples. After lapse of 10 minutes, the samples were unfolded, and presence or absence of the penetrant (degree of red) inside was visually confirmed to evaluate adhesion. The samples were evaluated based on the following criteria, and those samples which were evaluated to be C were determined to be failures. Tables 1 to 4 show the results.
A: No entry of the penetrant was confirmed.
B: No entry of the penetrant was confirmed on the inside of the package, but the penetrant was confirmed to have penetrated to part of the joint between the current output terminal and the terminal coating film.
C: Part of the package was confirmed to be dyed red on the inside thereof due to entry of the penetrant.
According to the present disclosure, a terminal coating resin film having good heat resistance, and a power storage device using the terminal coating resin film can be provided.
10 . . . Power storage device; 20 . . . Packaging material; 30 . . . Metal terminal (current output terminal); 40 . . . Terminal coating resin film; 40a . . . First layer; 40b . . . Second layer; 40c . . . Third layer; 100 . . . Power storage device.
Number | Date | Country | Kind |
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2018-121792 | Jun 2018 | JP | national |
This application is a continuation application filed under 35 U.S.C. § 111(a) claiming the benefit under 35 U.S.C. §§ 120 and 365(c) of International Patent Application No. PCT/JP2019/025221, filed on Jun. 25, 2019, which is based upon and claims the benefit of priority to Japanese Patent Application No. 2018-121792, filed on Jun. 27, 2018, the disclosures of which are all incorporated herein by reference in their entireties.
Number | Date | Country | |
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Parent | PCT/JP2019/025221 | Jun 2019 | US |
Child | 17110862 | US |