WO2019155940A1 - Accumulateur entièrement solide et son procédé de production - Google Patents

Accumulateur entièrement solide et son procédé de production Download PDF

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Publication number
WO2019155940A1
WO2019155940A1 PCT/JP2019/002977 JP2019002977W WO2019155940A1 WO 2019155940 A1 WO2019155940 A1 WO 2019155940A1 JP 2019002977 W JP2019002977 W JP 2019002977W WO 2019155940 A1 WO2019155940 A1 WO 2019155940A1
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Prior art keywords
solid
powder
secondary battery
laminate
state secondary
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PCT/JP2019/002977
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English (en)
Japanese (ja)
Inventor
健児 岡本
英之 福井
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日立造船株式会社
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Publication of WO2019155940A1 publication Critical patent/WO2019155940A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to an all solid state secondary battery and a method for manufacturing the same.
  • an all solid state secondary battery includes a positive electrode powder layer and a negative electrode powder layer, and a solid electrolyte layer disposed between the positive electrode powder layer and the negative electrode powder layer.
  • the powder laminate composed of the positive electrode powder layer, the solid electrolyte layer, and the negative electrode powder layer is formed by pressing a powder material, and the outer periphery thereof is covered with an insulating member.
  • the all-solid-state all-solid-state secondary battery has an advantage that safety is improved because no liquid is used.
  • Patent Document 1 Japanese Patent Application Laid-Open No. 2009-193728 discloses adhesion between a solid electrolyte layer and an insulating member (for example, an electrically insulating cylindrical frame). An all-solid-state secondary battery having an improved adhesion improvement region has been proposed.
  • the patent document 1 discloses an all-solid-state secondary battery for the purpose of suppressing an internal short circuit due to a gap between the cylindrical frame of the electrical insulating layer and the solid electrolyte layer, as described as the subject.
  • this all-solid-state secondary battery attempts to suppress voids formed on the side surfaces of the powder laminate (specifically, the solid electrolyte layer).
  • the all-solid-state secondary battery described in Patent Document 1 considers voids formed outside the powder laminate, but does not consider the interior of the powder laminate. For this reason, when the said all-solid-state secondary battery receives a vibration, an impact, etc., there exists a possibility that battery performance may fall because the inside of the said powder laminated body collapses. In particular, this tendency is remarkable when the inside of the solid electrolyte layer collapses in the powder laminate.
  • an object of the present invention is to provide an all-solid-state secondary battery that can prevent a decrease in battery performance and a method for manufacturing the same.
  • the all-solid-state secondary battery according to the first invention is an all-solid-state secondary battery comprising a powder laminate,
  • the powder laminate is A positive electrode powder layer and a negative electrode powder layer;
  • a solid electrolyte layer disposed between the positive electrode powder layer and the negative electrode powder layer, It further comprises an insulating pressing member that is disposed on the outer periphery of the solid electrolyte layer and presses the outer surface of the solid electrolyte layer in the powder laminate inward.
  • the all-solid-state secondary battery according to the second invention is characterized in that the pressing member in the all-solid-state secondary battery according to the first invention is arranged on the outer periphery of the positive electrode powder layer and / or the negative electrode powder layer, The outer surface of the powder layer and / or the negative electrode powder layer is pressed inward.
  • the all-solid-state secondary battery according to the third invention is the all-solid-state secondary battery according to the first or second invention, further comprising an insulating fibrous member in contact with the outer surface of the powder laminate.
  • the fibrous member includes a fibrous material,
  • the pressing member presses the outer surface of the powder laminate inward through the fibrous member.
  • the all-solid-state secondary battery which concerns on 4th invention contains the fibrous material in which the press member in the all-solid-state secondary battery which concerns on 1st or 2nd invention touches the outer surface of a powder laminated body. .
  • the manufacturing method of the all-solid-state secondary battery which concerns on 5th invention is a manufacturing method of the all-solid-state secondary battery which concerns on 1st or 2nd invention
  • the pressing member is an elastic member that presses the outer surface of the solid electrolyte layer in the powder laminate to the inside, Disposing the elastic member on the outer periphery of the solid electrolyte layer; Pressing the powder laminate and the elastic member in the thickness direction of the powder laminate to cause the elastic member to press the outer surface of the solid electrolyte layer inward.
  • the manufacturing method of the all-solid-state secondary battery which concerns on 6th invention is a manufacturing method of the all-solid-state secondary battery which concerns on 1st or 2nd invention, Comprising: The process of arrange
  • the pressing member presses at least the outer surface of the solid electrolyte layer in the powder laminate to the inside, so that at least the inside of the solid electrolyte layer in the powder laminate is unlikely to collapse. As a result, a decrease in battery performance can be prevented.
  • Embodiment 1 is a partially cutaway cross-sectional perspective view of an all solid state secondary battery according to Embodiment 1 of the present invention. It is sectional drawing in the case of being a member using an external pressure as a pressing member in the all-solid-state secondary battery. It is sectional drawing which shows the manufacturing method of the all-solid-state secondary battery, and shows the process of arrange
  • the all-solid-state secondary battery 1 includes a powder laminate 3.
  • the powder laminate 3 includes a positive electrode powder layer 4 and a negative electrode powder layer 6, and a solid electrolyte layer 5 disposed between the positive electrode powder layer 4 and the negative electrode powder layer 6.
  • the all-solid-state secondary battery 1 includes a positive electrode current collector 2 and a negative electrode current collector 7 disposed so as to sandwich the powder laminate 3 from the thickness direction as necessary, and a positive electrode current collector. And an insulating member 8 disposed between the body 2 and the negative electrode current collector 7 and outside the powder laminate 3.
  • the positive electrode current collector 2 is disposed in contact with the positive electrode powder layer 4, and the negative electrode current collector 7 is disposed in contact with the negative electrode powder layer 6.
  • the positive electrode current collector 2, the negative electrode current collector 7, and the insulating member 8 are not essential components, but are also members that protect the positive electrode powder layer 4 and the negative electrode powder layer 6.
  • the secondary battery 1 is preferably provided.
  • the powder laminate 3 is composed of powder without voids, that is, it is composed densely with powder. Such a powder laminate 3 is formed, for example, by pressing a powder material. As shown in FIG. 1 and FIG. 2, the outer surface 30 of the powder laminate 3 is formed along the thickness direction of the powder laminate 3, in other words, substantially parallel to the thickness direction (in production) And continuously formed.
  • the all-solid-state secondary battery 1 includes an insulating material disposed on the outer periphery of the powder laminate 3 and over the positive electrode powder layer 4, the solid electrolyte layer 5, and the negative electrode powder layer 6.
  • a pressing member 9 is provided. The pressing member 9 is not necessarily in contact with the powder laminate 3 as long as it is disposed on the outer periphery of the powder laminate 3. However, the pressing member 9 needs to extend over the positive electrode powder layer 4, the solid electrolyte layer 5, and the negative electrode powder layer 6.
  • the pressing member 9 extends from a position where the positive electrode powder layer 4 is extended in a direction perpendicular to the thickness direction to a position where the negative electrode powder layer 6 is extended in a direction perpendicular to the thickness direction. , Need to reach.
  • the powder laminate 3 when the powder laminate 3 is not pressed inward, it easily breaks when subjected to vibration or impact. In order to prevent this, the outer surface 30 of the powder laminate 3 is pressed inward by the pressing member 9.
  • the pressing of the outer side surface 30 by the pressing member 9 is not limited to a direct one as shown in FIGS. 1 and 2 but indirectly through another member 11 as shown in FIG. 7 (described later). It may be a natural one.
  • the pressing member 9 is disposed on the outer periphery of the powder laminate 3 and over the positive electrode powder layer 4, the solid electrolyte layer 5, and the negative electrode powder layer 6, and the outer surface 30 is disposed on the powder laminate 3. Any member that presses inward may be used, and examples thereof include the elastic member 9 and / or a member that uses external pressure.
  • the elastic member 9 When the pressing member 9 is the elastic member 9, the elasticity of the elastic member 9 is used for pressing the outer surface 30.
  • the outer surface 30 is pressed by the elastic force of the elastic member 9, specifically, the force of the elastic member 9 expanding or moving to the inside of the powder laminate 3.
  • the elastic member 9 may be a member that presses the outer surface 30 with a force that is compressed in the thickness direction to expand in a direction orthogonal to the thickness direction, that is, a Poisson effect. Good.
  • the preferred elastic member 9 is in contact with the outer surface 30 in its entirety and presses the entire outer surface 30. Thereby, even if the said powder laminated body 3 receives a vibration, an impact, etc., it becomes difficult to collapse.
  • the elastic member 9 When the pressing member 9 is the elastic member 9, the elastic member 9 preferably has an elastic coefficient of 20 MPa or less so that the elastic member 9 presses the outer surface 30 more appropriately.
  • the all-solid-state secondary battery 1 includes the powder laminate 3, the positive electrode current collector 2, and the negative electrode current collector.
  • a laminate pack 10 (a bag-like flexible exterior body)
  • the laminate pack 10 accommodates the battery bodies 2, 3, 7 to 9 therein, and the interior is sucked by a vacuum pump P or the like and sealed. For this reason, the laminate pack 10 receives pressure such as atmospheric pressure (ie, external pressure F) from the outside due to the pressure difference F between the inside and the outside.
  • the external pressure F presses the outer surface 30 of the powder laminate 3 inward through the pressing member 9 shown in FIG.
  • the pressing member 9 shown in FIG. 3 presses the outer surface 30 of the powder laminate 3 inward by the pressure difference F between the inside and the outside of the laminate pack 10.
  • the pressing member 9 is a member that uses the external pressure F
  • the member has an extremely low elastic modulus such as 2 MPa or less in order to sufficiently transmit the external pressure F to the outer surface 30 of the powder laminate 3. It is preferably an elastic member.
  • the positive electrode current collector 2 and the negative electrode current collector 7 copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn) ), Aluminum (Al), germanium (Ge), indium (In), lithium (Li), tin (Sn), thin plates and foils made of these alloys, etc. Used.
  • the thin plate member and the foil member have a thickness in the range of 5 ⁇ m to 100 ⁇ m.
  • the positive electrode current collector 2 and the negative electrode current collector 7 may have a surface subjected to a roughening treatment from the viewpoint of improving adhesion to the powder laminate 3 composed of powder. preferable.
  • the roughening process is a process for increasing the surface roughness by etching or the like.
  • the insulating member 8 is an insulating sheet made of a polymer material such as a PET film.
  • the positive electrode powder layer 4 and the negative electrode powder layer 6 are formed of a positive electrode active material and a negative electrode active material that secure an electron conduction path between particles in order to exchange electrons, and a solid electrolyte having ion conductivity. It is a layer made of a mixed material mixed at a ratio. Thus, by mixing the positive electrode active material and the negative electrode active material with a solid electrolyte having lithium ion conductivity, ion conductivity can be imparted in addition to electron conductivity, and an ion conduction path can be secured between particles. .
  • the positive electrode powder layer 4 and the negative electrode powder layer 6 may be layers made of only the positive electrode active material and the negative electrode active material.
  • the positive electrode active material suitable for the positive electrode powder layer 4 is not particularly limited as long as it can insert and release lithium ions.
  • lithium-nickel composite oxide LiNi x M 1-x O 2
  • lithium cobaltate LiCoO 2
  • lithium nickelate LiNiO 2
  • lithium-nickel-cobalt-aluminum composite oxide LiNi 0.8 Co 0.15 Al 0.05 O 2 , NCA-based layered oxide
  • lithium manganate such as spinel type lithium manganate LiMn 2 O 4
  • Li-rich composite oxide Li 2 MnO 3 —LiMO 2
  • Examples of compounds other than oxides include olivine compounds (LiMPO 4 ), sulfur-containing compounds (Li 2 S, etc.), and the like.
  • M represents a transition metal.
  • a positive electrode active material can be used individually by 1 type or in combination of 2 or more types. From the viewpoint of easily obtaining a high capacity, a lithium-containing oxide containing at least one selected from the group consisting of Co, Ni and Mn is preferable.
  • the lithium-containing oxide may further contain a typical metal element such as Al.
  • the positive electrode active material may be coated with a coating material on the surface of the active material from the viewpoint of improving rate characteristics.
  • a coating material Li 4 Ti 5 O 12 , LiTaO 3 , Li 4 NbO 3 , LiAlO 2 , Li 2 ZrO 3 , Li 2 WO 4 , Li 2 TiO 3 , Li 2 B 4 O 7 , Examples thereof include Li 3 PO 4 , Li 2 MoO 4 , LiBO 2 , alumina (Al 2 O 3 ), and carbon (C).
  • a negative electrode active material suitable for the negative electrode powder layer 6 a mixed material of a negative electrode active material and a lithium ion conductive solid electrolyte, or a negative electrode active material is used alone.
  • the negative electrode active material is not particularly limited as long as lithium ions can be inserted and desorbed, and known negative electrode active materials used in all solid state batteries can be used.
  • Examples of the negative electrode active material include carbonaceous materials capable of inserting and desorbing lithium ions, and simple metals, semimetals, alloys, and compounds capable of inserting and desorbing lithium ions.
  • Examples of the carbonaceous material include graphite (natural graphite, artificial graphite, etc.), hard carbon, amorphous carbon, and the like.
  • Examples of simple metals and metalloids and alloys include lithium metal, alloys, and Si.
  • Examples of the compound include oxides, sulfides, nitrides, hydrates, silicides (such as lithium silicide), and the like.
  • Examples of the oxide include titanium oxide and silicon oxide.
  • a negative electrode active material may be used individually by 1 type, and may be used in combination of 2 or more type. For example, silicon oxide and a carbonaceous material may be used in combination.
  • Solid electrolytes are roughly classified into organic polymer electrolytes (also referred to as organic solid electrolytes), inorganic inorganic solid electrolytes, and the like, and any of them may be used as the solid electrolyte.
  • organic solid electrolytes are roughly classified into oxide-based materials and sulfide-based materials, and any of them may be used.
  • the inorganic solid electrolyte can be appropriately selected from crystalline or amorphous ones. That is, the solid electrolyte can be appropriately selected from materials made of organic compounds, inorganic compounds, or mixtures thereof.
  • examples of materials that can be used as the solid electrolyte include lithium ion conductive solid electrolytes and sulfide-based inorganic solid electrolytes that are known to have higher ion conductivity than other inorganic compounds. is there.
  • lithium-containing metal oxides such as one or more metals
  • Li 2 —SiO 2 and Li 2 —SiO 2 —P 2 O 5 Li x P y O 1 lithium-containing metal nitride such as -z N 2, Li 2 S- P 2 S 5 based, Li 2 S-SiS 2 system, Li 2 S-B 2 S 3 system, Li 2 S-GeS 2 system, Li 2 S-SiS 2 -LiI system, Li 2 S-SiS 2 -Li 3 PO 4 based, Li 2 S-Ge 2 S 2 system, Li 2 S-GeS 2 -P 2 S 5 based, Li 2 S-GeS 2 lithium-containing sulfide-based glass such -ZnS-based, and PEO (polyethylene oxide), PVDF (polyvinylidene fluoride), lithium phosphate (Li 3 PO 4), lithium-containing transition metal oxide such as lithium titanium oxide
  • PEO polyethylene oxide
  • PVDF polyvinylidene
  • sulfide sulfide-based inorganic solid electrolyte
  • the sulfide for example, one or two or more sulfides including Li 2 S and at least one element selected from the group consisting of Group 13 elements, Group 14 elements, and Group 15 elements of the periodic table The thing containing these is preferable.
  • the group 13-15 element of the periodic table is not particularly limited, and examples thereof include P, Si, Ge, As, Sb, Al, and the like. P, Si, Ge are preferable, and P Is preferred. A sulfide containing these elements (particularly P) and Li is also preferable.
  • the solid electrolyte suitable for the solid electrolyte layer 5 may be the same as or different from the solid electrolyte used in the positive electrode powder layer 4 and the negative electrode powder layer 6.
  • the positive electrode active material, the negative electrode active material, and the solid electrolyte are not limited to the materials described above, and those that are common in the field of batteries can also be used.
  • the insulating pressing member 9 is not particularly limited, but for example, the elastic member 9 is employed as described above.
  • Such an elastic member 9 is made of rubber or elastomer.
  • the powder laminate 3 and the insulating member 8 are arranged in advance on the upper surface of the positive electrode current collector 2 (or the negative electrode current collector 7).
  • the powder laminate 3 may be one that has already been pressurized in the thickness direction, or may be one before being pressed that is scheduled to be pressurized in the thickness direction later.
  • the elastic member 9 is disposed on the upper surface of the positive electrode current collector 2 (or the negative electrode current collector 7) and on the outer periphery of the powder laminate 3. The elastic member 9 is pressed in the thickness direction later, thereby pressing the outer side surface 30 of the powder laminate 3 inward with a force due to the Poisson effect.
  • the thickness of the elastic member 9 before being pressed in the thickness direction and the material of the elastic member 9 are determined so that this force is appropriate.
  • the elastic member 9 before being pressed in the thickness direction is thicker than the powder laminate 3, for example, as shown in FIG. Further, when the elastic member 9 is disposed on the outer periphery of the powder laminate 3, the elastic member 9 does not contact the powder laminate 3 in order not to collapse by rubbing the outer surface 30 of the powder laminate 3. It is preferable that they are arranged as described above.
  • the negative electrode current collector 7 (or the positive electrode current collector 2) is disposed on the powder laminate 3 and the elastic member 9, and the positive electrode current collector 2 and the negative electrode current collector 7 are arranged. In a direction approaching each other. By this pressurization, the elastic member 9 is compressed in the thickness direction. However, the elastic member 9 tries to expand in the direction perpendicular to the thickness direction by the Poisson effect. Press the entire surface of 30 inward.
  • the pressing member 9 does not necessarily have to press the outer surface 30 of the powder laminate 3.
  • the laminate pack 10 is sealed while sucking the inside of the laminate pack 10 with a vacuum pump P or the like.
  • the laminate pack 10 receives pressure such as atmospheric pressure (ie, external pressure F) from the outside due to the pressure difference F between the inside and the outside.
  • external pressure F the pressure in the direction orthogonal to the thickness direction presses the powder laminate 3 inward through the pressing member 9.
  • the pressing member 9 extending from the positive electrode powder layer 4 to the negative electrode powder layer 6 presses the outer surface 30 of the powder laminate 3 inward.
  • the interior of the powder laminate 3 is less likely to collapse, and as a result, it is possible to prevent a decrease in battery performance.
  • the pressing member 9 extending from the positive electrode powder layer 4 to the negative electrode powder layer 6 is disposed on the outer periphery of the powder laminate 3, the positive and negative electrodes are formed by the collapse of the powder laminate 3 from the outer surface 30. A short circuit can be prevented.
  • the elastic member 9 that presses the entire outer surface 30 of the powder laminate 3 as the pressing member 9 expands following the contraction of the powder laminate 3. As a result, no short-circuit between the positive and negative electrodes due to the collapse of the powder laminate 3 from the outer surface 30 can be prevented.
  • the all-solid-state secondary battery 1 according to Embodiment 2 of the present invention includes an insulating fibrous member 11 disposed between the pressing member 9 and the powder laminate 3, as shown in FIG. It is.
  • the fibrous member 11 of the all-solid-state secondary battery 1 according to Embodiment 2 of the present invention includes a fibrous material, is in contact with the outer surface 30 of the powder laminate 3, and is disposed on the inner periphery of the pressing member 9. Is done.
  • the fibrous member 11 is a member that can entangle powder with the fibrous material. For this reason, in the all-solid-state secondary battery 1, even if the outer surface 30 of the powder laminate 3 collapses, the collapsed powder is entangled with the fibrous member 11, so that the positive and negative electrodes are not short-circuited.
  • the pressing member 9 does not contact the powder laminate 3, but presses the powder laminate 3 through the fibrous member 11.
  • the insulating fibrous member 11 is not particularly limited, and for example, glass fiber, alumina fiber or sponge-like member (sponge) is used.
  • the manufacturing method of the all-solid-state secondary battery 1 according to Embodiment 2 of the present invention is the same as the manufacturing method of the all-solid-state secondary battery 1 according to Embodiment 1 except that the pressing member 9 is provided on the outer periphery of the powder laminate 3.
  • the step of arranging is replaced with a step of arranging the pressing member 9 and the fibrous member 11 on the outer periphery of the powder laminate 3.
  • the same effects as those of the first embodiment can be obtained, and the outer surface 30 of the powder laminate 3 is collapsed.
  • the collapsed powder is entangled with the fibrous member 11, it is possible to further prevent a short circuit between the positive and negative electrodes due to the collapse of the powder laminate 3 from the outer surface 30.
  • the pressing member 91 also has the function of the fibrous member 11 according to Embodiment 2.
  • the pressing member 91 of the all-solid-state secondary battery 1 according to Embodiment 3 of the present invention is in contact with the outer surface 30 of the powder laminate 3 and at least a portion that is in contact with the outer surface 30. It contains a fibrous material. Of course, as shown in FIG. 8, all of the pressing member 91 may be a fibrous material.
  • the same effects as those of the second embodiment can be obtained, and it is not necessary to provide the separate fibrous member 11. Therefore, the configuration can be made simpler than that of the second embodiment.
  • the all-solid-state secondary battery 1 according to Embodiment 4 of the present invention is an elastic member 9 in which the pressing member 9 presses only the solid electrolyte layer 5 in the powder laminate 3.
  • the elastic member 9 is disposed between the upper and lower outer peripheral members 16 and 14 on the upper and lower sides.
  • the upper outer peripheral member 16 and the lower outer peripheral member 14 are made of resin or ceramic.
  • the elastic member 9 before being pressed in the thickness direction is thicker than the solid electrolyte layer 5, for example, as shown in FIG. Further, when the elastic member 9 is disposed on the outer periphery of the powder laminate 3, the elastic member 9 does not contact the powder laminate 3 in order not to collapse by rubbing the outer surface 30 of the powder laminate 3. It is preferable that they are arranged as described above. Thereafter, as shown in FIG. 10, the negative electrode current collector 7 (or the positive electrode current collector 2) is arranged on the powder laminate 3 and the upper outer peripheral member 16, and the positive electrode current collector 2 and the negative electrode current collector are arranged. 7 is pressurized in a direction approaching each other.
  • the elastic member 9 is compressed in the thickness direction, but tries to expand in the direction perpendicular to the thickness direction due to the Poisson effect, and the solid electrolyte in the powder laminate 3 is subjected to the expansion force.
  • the entire outer surface 30 of the layer 5 is pressed inward.
  • the same effects as those of the first embodiment can be obtained, and the amount of the elastic member 9 can be further reduced. .
  • the all-solid-state secondary battery 1 according to the fifth embodiment of the present invention corresponds to the lower outer peripheral member 14 instead of using the lower outer peripheral member 14 in the fourth embodiment.
  • the insulating member 8 is protruded inward to the position where it does.
  • the fifth embodiment of the present invention is the same as the fourth embodiment.
  • the insulating member 8 may be protruded inward to a position corresponding to the upper outer peripheral member 16.
  • the all-solid-state secondary battery 1 and the manufacturing method thereof according to the fifth embodiment the same effect as that of the fourth embodiment is obtained, and the lower outer peripheral member 14 or the upper outer peripheral member 16 is not required. Therefore, the number of parts can be reduced.
  • the all solid state secondary battery 1 according to Embodiment 6 of the present invention corresponds to the upper outer periphery member 16 in Embodiment 4 instead of using the upper outer periphery member 16.
  • the elastic member 9 has a thickness up to the position to be.
  • the sixth embodiment of the present invention is the same as the fourth embodiment.
  • the elastic member 9 may have a thickness up to a position corresponding to the lower outer peripheral member 14.
  • the all-solid-state secondary battery 1 and the manufacturing method thereof according to the sixth embodiment the same effect as that of the fourth embodiment is obtained, and the upper outer peripheral member 16 or the lower outer peripheral member 14 is unnecessary. Therefore, the number of parts can be reduced.
  • the pressing member 9 is solid with the positive electrode powder layer 4 and the negative electrode powder layer 6 of the powder laminate 3.
  • An elastic member 9 that presses the electrolyte layer 5 with a different force.
  • the elastic member 9 disposed on the outer periphery includes an upper portion 96, a lower portion 94, and a middle portion 95.
  • the upper portion 96 and the lower portion 94 are made of a material having an elastic coefficient higher than that of the middle portion 95, so that the negative electrode powder layer 6 and the positive electrode powder layer 4 can be formed with a force smaller than that of the middle portion 95. Press.
  • the middle portion 95 is made of a material having an elastic coefficient lower than that of the upper portion 96 and the lower portion 94, thereby pressing the solid electrolyte layer 5 with a force larger than that of the upper portion 96 and the lower portion 94.
  • the solid electrolyte layer 5 that leads to a larger deterioration in battery performance due to the collapse of the inside is formed into the positive electrode powder layer 4 and the negative electrode. Since the pressing is performed with a force larger than that of the powder layer 6, it is possible to effectively prevent the battery performance from being lowered.
  • the pressing member 9 is solid with the positive electrode powder layer 4 and the negative electrode powder layer 6 of the powder laminate 3.
  • the elastic member 9 presses the electrolyte layer 5 with a different force, but the configuration is different from that of the seventh embodiment.
  • the elastic member 9 disposed on the outer periphery has a narrow cross section at a portion where the positive electrode powder layer 4 and the negative electrode powder layer 6 are pressed, and a cross section at a portion where the solid electrolyte layer 5 is pressed. It is wide.
  • the positive electrode powder layer 4 and the negative electrode powder layer 6 are pressed by the elastic member 9 with a force smaller than that of the solid electrolyte layer 5.
  • the solid electrolyte layer 5 is pressed by the elastic member 9 with a larger force than the positive electrode powder layer 4 and the negative electrode powder layer 6.
  • the same effects as those of the seventh embodiment can be obtained, and the upper portion 96 and the lower portion 94 of the elastic member 9 are unnecessary. Therefore, the number of parts can be reduced.
  • the pressing member 9 is disposed on the outer periphery of the powder laminate 3 from the positive electrode powder layer 4 to the negative electrode powder layer 6, but at least the solid electrolyte layer It is only necessary to dispose at least the solid electrolyte layer 5 on the inner side.
  • the pressing member 9 presses many parts of the powder laminate 3, the inside of the powder laminate 3 is more unlikely to collapse, and as a result, the battery performance can be further prevented from being deteriorated.
  • the positive electrode current collector 2, the negative electrode current collector 7, and the insulating member 8 have been described.
  • positioned may be sufficient.
  • the insulating pressing member 9 also serves as the insulating member 8, so that the pressing member 9 occupies the area of reference numeral 8 in FIGS. 1 to 3, 7 and 8. It is preferable that
  • the all-solid-state secondary batteries 1 of Embodiments 1 to 8 are shown in FIG. 2 as having a rectangular shape in plan view, the present invention is not limited to this.
  • the planar view may be a polygonal shape or a circular shape.
  • the laminate pack 10 has been described as an example of a bag-shaped flexible exterior body.
  • the present invention is not limited thereto, and the bag-shaped flexible exterior body is not limited thereto. Any body is acceptable.
  • the first to eighth embodiments are examples in all respects and are not restrictive.
  • the scope of the present invention is defined by the terms of the claims, rather than the description above, and is intended to include any modifications within the scope and meaning equivalent to the terms of the claims.
  • the configuration other than the configuration described as the first invention in “Means for Solving the Problems” is an arbitrary configuration, and can be appropriately deleted and changed. It is.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Inorganic Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Secondary Cells (AREA)
  • Sealing Battery Cases Or Jackets (AREA)

Abstract

L'invention concerne un accumulateur entièrement solide (1) comprenant un stratifié de poudre (3). Le stratifié de poudre (3) comporte : une couche de poudre d'électrode positive (4), une couche de poudre d'électrode négative (6) et une couche d'électrolyte solide (5) disposée entre la couche de poudre d'électrode positive (4) et la couche de poudre d'électrode négative (6). L'accumulateur entièrement solide (1) comprend un élément de pression isolant (9) qui est disposé au niveau de la périphérie externe de la couche d'électrolyte solide (5) et est destiné à presser vers l'intérieur au moins la surface externe (30) de la couche d'électrolyte solide (5) du stratifié de poudre (3).
PCT/JP2019/002977 2018-02-08 2019-01-29 Accumulateur entièrement solide et son procédé de production WO2019155940A1 (fr)

Applications Claiming Priority (2)

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JP2018020579A JP7133316B2 (ja) 2018-02-08 2018-02-08 全固体二次電池およびその製造方法
JP2018-020579 2018-02-08

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Publication number Priority date Publication date Assignee Title
WO2020090736A1 (fr) * 2018-10-29 2020-05-07 株式会社村田製作所 Batterie à électrolyte solide

Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0513102A (ja) * 1991-07-03 1993-01-22 Matsushita Electric Ind Co Ltd 全固体電気化学素子の製造法
JP2000106154A (ja) * 1998-09-28 2000-04-11 Matsushita Electric Ind Co Ltd 全固体電池およびその製造法
WO2010131321A1 (fr) * 2009-05-11 2010-11-18 トヨタ自動車株式会社 Batterie à électrolyte solide et son procédé de fabrication
JP2012069248A (ja) * 2010-09-21 2012-04-05 Hitachi Zosen Corp 全固体電池の製造方法
WO2012164723A1 (fr) * 2011-06-02 2012-12-06 トヨタ自動車株式会社 Procédé de formation d'une cellule entièrement à semi-conducteurs
JP2016152204A (ja) * 2015-02-19 2016-08-22 三星電子株式会社Ｓａｍｓｕｎｇ Ｅｌｅｃｔｒｏｎｉｃｓ Ｃｏ．，Ｌｔｄ． 固体電池及びその製造方法

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH0513102A (ja) * 1991-07-03 1993-01-22 Matsushita Electric Ind Co Ltd 全固体電気化学素子の製造法
JP2000106154A (ja) * 1998-09-28 2000-04-11 Matsushita Electric Ind Co Ltd 全固体電池およびその製造法
WO2010131321A1 (fr) * 2009-05-11 2010-11-18 トヨタ自動車株式会社 Batterie à électrolyte solide et son procédé de fabrication
JP2012069248A (ja) * 2010-09-21 2012-04-05 Hitachi Zosen Corp 全固体電池の製造方法
WO2012164723A1 (fr) * 2011-06-02 2012-12-06 トヨタ自動車株式会社 Procédé de formation d'une cellule entièrement à semi-conducteurs
JP2016152204A (ja) * 2015-02-19 2016-08-22 三星電子株式会社Ｓａｍｓｕｎｇ Ｅｌｅｃｔｒｏｎｉｃｓ Ｃｏ．，Ｌｔｄ． 固体電池及びその製造方法

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