WO2015147122A1 - 全固体二次電池 - Google Patents
全固体二次電池 Download PDFInfo
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- WO2015147122A1 WO2015147122A1 PCT/JP2015/059286 JP2015059286W WO2015147122A1 WO 2015147122 A1 WO2015147122 A1 WO 2015147122A1 JP 2015059286 W JP2015059286 W JP 2015059286W WO 2015147122 A1 WO2015147122 A1 WO 2015147122A1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—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
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
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- 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
-
- 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
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/60—Other road transportation technologies with climate change mitigation effect
- Y02T10/70—Energy storage systems for electromobility, e.g. batteries
Definitions
- the present invention relates to an all solid state secondary battery.
- an all-solid-state lithium ion secondary battery in order to reduce the grain boundary resistance of the electrode material made of a granular material, it is pressure-molded with the electrode material sandwiched between the positive electrode current collector and the negative electrode current collector. .
- the sulfide inorganic solid electrolyte when a sulfide inorganic solid electrolyte is used as the electrode material, the sulfide inorganic solid electrolyte has high binding force and ductility, so that the adhesion between the particles in the electrode material is improved by the pressure molding. Further, since the sulfide inorganic solid electrolyte has a lower ionic conductivity than the oxide inorganic solid electrolyte, the above-described pressure molding is important. Furthermore, by using a material having high adhesion for the positive electrode current collector and the negative electrode current collector, the electrical resistance between the positive electrode current collector and the negative electrode current collector and the electrode material is reduced.
- an all-solid-state lithium ion secondary battery using a sulfide inorganic solid electrolyte as an electrode material warps to the positive electrode side or the negative electrode side by the pressure molding. This warping is not a problem when the maximum outer length of the all-solid-state lithium ion secondary battery is small, but the amount of bending is not a problem when the maximum outer length is large. If this warpage is corrected, the electrode material may be cracked.
- a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector are laminated on both sides of the positive electrode current collector.
- a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector are laminated on both sides of the positive electrode current collector.
- the all-solid-state secondary battery is a single cell, it has the advantages that the manufacturing process is shortened and the wiring is simplified.
- the all solid lithium ion secondary battery described in Patent Document 1 is premised on being a multilayer cell. In other words, the all-solid lithium ion secondary battery has a problem that it cannot be made into a single cell.
- an object of the present invention is to provide a single-cell all-solid-state secondary battery capable of suppressing warpage.
- an all-solid-state secondary battery of the present invention is provided with a positive electrode layer and a negative electrode layer that are disposed and pressed on a positive electrode current collector and a negative electrode current collector, respectively,
- An all-solid-state secondary battery comprising a solid electrolyte layer disposed between a positive electrode layer and a negative electrode layer, The positive electrode layer and the negative electrode layer have a sulfide inorganic solid electrolyte, The positive electrode current collector and the negative electrode current collector have a peel strength of 0.2 N / mm or more from the sulfide inorganic solid electrolyte by a peel test.
- the all-solid-state secondary battery of the present invention according to claim 2 is the all-solid-state secondary battery of the invention according to claim 1, wherein the solid electrolyte layer is made of a sulfide inorganic solid electrolyte.
- the all solid state secondary battery of the present invention according to claim 3 is the all solid state secondary battery according to claim 1 or 2, wherein the positive electrode current collector is tin or etched aluminum.
- the negative electrode current collector is roughened copper.
- the warpage of the positive electrode current collector and the positive electrode layer and the warpage of the negative electrode current collector and the negative electrode layer are offset in a single cell. be able to.
- an all solid state secondary battery according to an embodiment of the present invention will be described with reference to the drawings.
- an all-solid secondary battery an all-solid secondary battery using a lithium ion conductive material as a solid electrolyte, that is, an all-solid lithium ion secondary battery will be described.
- a lithium ion conductive solid electrolyte layer (hereinafter simply referred to as a solid electrolyte layer 3) is disposed (laminated) between the positive electrode layer 2 and the negative electrode layer 4.
- the positive electrode current collector 1 is disposed on the surface of the positive electrode layer 2 opposite to the solid electrolyte layer 3
- the negative electrode current collector 5 is disposed on the surface of the negative electrode layer 4 opposite to the solid electrolyte layer 3. (Laminated).
- the positive electrode layer 2 and the negative electrode layer 4 are layers to be electrodes, that is, electrode layers.
- the said positive electrode layer 2 and the negative electrode layer 4 are mentioned later in detail, all have a sulfide inorganic solid electrolyte.
- the positive electrode layer 2, the solid electrolyte layer 3, and the negative electrode layer 4 are all formed from a powder material.
- the insulating film 6 may be disposed on the outer periphery of the positive electrode layer 2.
- the positive electrode layer 2 disposed on the surface of the positive electrode current collector 1 is pressure-molded, the positive electrode layer 2 is compressed in the thickness (lamination) direction as shown in FIG. Although it tries to expand in the width direction, it receives the frictional force F from the positive electrode current collector 1 in the opposite direction of the width direction and cannot expand in the width direction. For this reason, a residual stress that tends to expand in the width direction is generated in the positive electrode layer 2. However, as shown in FIG. 4, the positive electrode layer 2 that has been subjected to pressure molding is released from the residual stress and tends to expand in the width direction.
- the peel strength of the positive electrode current collector 1 from the sulfide inorganic solid electrolyte by the peel test is less than 0.2 N / mm
- the positive electrode current collector 1 and the positive electrode layer 2 (having the sulfide inorganic solid electrolyte) Low adhesion.
- the positive electrode layer 2 expands while sliding on the surface of the positive electrode current collector 1, and thus does not affect the shape of the positive electrode current collector 1.
- the peel strength of the positive electrode current collector 1 from the sulfide inorganic solid electrolyte by the peel test is 0.2 N / mm or more, the adhesion between the positive electrode current collector 1 and the positive electrode layer 2 is high.
- the positive electrode layer 2 expands while biting into the surface of the positive electrode current collector 1, so that the positive electrode current collector 1 is warped.
- the contents described above are not only for the positive electrode current collector 1 and the positive electrode layer 2 but also for the negative electrode current collector 5 and the negative electrode layer 4 although not shown.
- the present invention cancels the warpage of the positive electrode current collector 1 and the positive electrode layer 2 and the warpage of the negative electrode current collector 5 and the negative electrode layer 4. It is intended to suppress warping as.
- the positive electrode layer 2 a mixture of a positive electrode active material and a lithium ion conductive solid electrolyte is used.
- the weight ratio of the positive electrode active material and the lithium ion conductive solid electrolyte in the mixture is, for example, 7: 3.
- the positive electrode active material includes lithium-nickel composite oxide (LiNi x M 1-x O 2 ; M is Co, Al, Mn, V, Cr, Mg, Ca, Ti, Zr, Nb, Mo, and W Among these, materials usually used for the positive electrode active material in the battery field, such as at least one element), lithium cobaltate (LiCoO 2 ), lithium nickelate (LiNiO 2 ), lithium manganate (LiMnO 2 ), are used.
- the negative electrode layer 4 a mixture of a negative electrode active material and a lithium ion conductive solid electrolyte is used.
- the weight ratio of the negative electrode active material and the lithium ion conductive solid electrolyte in the mixture is, for example, 6: 4.
- the negative electrode active material includes natural graphite, artificial graphite, carbon materials such as graphite carbon fiber or resin-fired carbon, silicon, tin, lithium, oxide, sulfide, nitride, alloy, powder, foil, etc. Regardless of the shape, a material usually used for a negative electrode active material in the battery field is used.
- the lithium ion conductive solid electrolytes of the positive electrode layer 2, the solid electrolyte layer 3, and the negative electrode layer 4 are usually used in the field of lithium ion batteries, materials composed of organic compounds, inorganic compounds, and both organic and inorganic compounds. The materials that are used are used. Further, among inorganic compounds, for example, a sulfide system such as Li 2 S—P 2 S 5 is superior in ion conductivity as compared with other inorganic compounds.
- the positive electrode current collector 1 and the negative electrode current collector 5 are made of untreated surface tin, etched aluminum having a large number of sponge-like pores formed on the surface by etching (see FIG. 8), or a pyramidal shape on the surface. For example, roughened copper (see FIG. 9) in which many low pyramids are formed is used. Moreover, these are a plate-shaped body, a foil-shaped body, a film-formed body, or a metal foil composite. This metal foil composite is a composite obtained by applying a surface coat to a metal foil. For example, a carbon coat is applied to the surface of a stainless steel foil.
- the positive electrode current collector 1 and the negative electrode current collector 5 may be the same or different.
- the peel strength from the sulfide inorganic solid electrolyte by the peel test is high (0.2 N / mm or more). Become.
- Li 2 S—P 2 S 5 layer L (not the layer made of the same material as the positive electrode layer 2 or the negative electrode layer 4) is used as the layer constituting the test piece of the peel test will be described.
- the binding force between the powders becomes small. This binding force is smaller than the adhesion between the electrode mixture and the current collectors 1 and 5. For this reason, when a layer made of an electrode mixture is used as the layer constituting the test piece, the layer made of the electrode mixture breaks (also referred to as delamination) in the peel test. Separation with current collectors 1 and 5 does not occur. Therefore, the value measured by the peel test is not the peel strength between the layer made of the electrode mixture and the current collectors 1 and 5, but the delamination strength of the layer made of the electrode mixture.
- the peel test is a 90 ° peel test, it is intended to peel in the thickness (lamination) direction.
- the layer which consists of electrode compound materials peels in a peel test.
- an actual all solid lithium ion secondary battery tends to expand in the width direction instead of the thickness (lamination) direction, and thus the electrode material does not delaminate. Therefore, it is considered that even if any of the layers made of the electrode mixture and the Li 2 S—P 2 S 5 layer L is in close contact with the current collectors 1, 5, it has an equivalent adhesion force.
- the value obtained by dividing the average value of the load obtained by the above measurement by the length in the short direction of the test piece is the peel strength by the peel test (more precisely, 90 ° peel test).
- the positive electrode layer 2 is formed on the surface of the positive electrode current collector 1 by a dry film forming method.
- the solid electrolyte layer 3 is formed on the surface of the positive electrode layer 2 opposite to the positive electrode current collector 1 by a dry film forming method.
- the negative electrode layer 4 is formed on the surface of the solid electrolyte layer 3 opposite to the positive electrode layer 2 by a dry film forming method.
- the negative electrode collector 5 is laminated
- the warpage of the positive electrode current collector 1 and the positive electrode layer 2 and the warpage of the negative electrode current collector 5 and the negative electrode layer 4 are offset in a single cell. Even if there is, the warp can be suppressed.
- the positive electrode layer 2 is a 50 mm square, LiNi 0.8 Co 0.15 Al 0.05 O 2 (particle size: 6 ⁇ m) is used as the positive electrode active material of the positive electrode layer 2, and the lithium ion conductive solid of the positive electrode layer 2 Li 2 S (80 mol%)-P 2 S 5 (20 mol%) was used as the electrolyte.
- the solid electrolyte layer 3 was 54 mm square, and Li 2 S (80 mol%)-P 2 S 5 (20 mol%) was used for the solid electrolyte layer 3.
- the negative electrode layer 4 is 54 mm square, graphite (particle size 25 ⁇ m) is used as the negative electrode active material of the negative electrode layer 4, and Li 2 S (80 mol%)-P 2 S is used as the lithium ion conductive solid electrolyte of the negative electrode layer 4. 5 (20 mol%) was used.
- Comparative Example 2 Stainless steel foil (material with low adhesion) was used for the positive electrode current collector, and roughened copper foil (material with high adhesion) was used for the negative electrode current collector. According to the all-solid-state lithium ion secondary battery according to Comparative Example 2, although not shown, the amount of bending due to warpage was the same as that of Comparative Example 1.
- Etched aluminum (a material with high adhesion) was used for the positive electrode current collector 1
- roughened copper foil (a material with high adhesion) was used for the negative electrode current collector 5. According to the all-solid-state lithium ion secondary battery of Example 1, the amount of bending due to warpage could be suppressed to 5 to 6 mm, which is about 1/3 of the comparative example (FIG. 14).
- Tin highly adhesive material
- roughened copper foil highly adhesive material
- the peel strength of the body 5 from the sulfide inorganic solid electrolyte by the peel test may be 0.2 N / mm or more.
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Abstract
Description
上記正極層および負極層は、硫化物無機固体電解質を有し、
上記正極集電体および負極集電体は、ピール試験による硫化物無機固体電解質との剥離強度が0.2N/mm以上であるものである。
負極集電体は、粗化銅であるものである。
(1)正極層2を50mm角とし、正極層2の正極活物質にLiNi0.8Co0.15Al0.05O2(粒径6μm)を用い、正極層2のリチウムイオン伝導性固体電解質にLi2S(80mol%)-P2S5(20mol%)を用いた。
(2)固体電解質層3を54mm角とし、固体電解質層3にLi2S(80mol%)-P2S5(20mol%)を用いた。
(3)負極層4を54mm角とし、負極層4の負極活物質にグラファイト(粒径25μm)を用い、負極層4のリチウムイオン伝導性固体電解質にLi2S(80mol%)-P2S5(20mol%)を用いた。
正極集電体にエッチドアルミニウム(密着性の高い材料)を用い、負極集電体に電解銅箔(密着性の低い材料)を用いた。本比較例1に係る全固体リチウムイオン二次電池によると、反りによる湾曲量が15~20mmとなった(図13)。
正極集電体にステンレス箔(密着性の低い材料)を用い、負極集電体に粗化銅箔(密着性の高い材料)を用いた。本比較例2に係る全固体リチウムイオン二次電池によると、図示しないが、反りによる湾曲量が上記比較例1と同様になった。
Claims (3)
- 正極集電体および負極集電体にそれぞれ配置されるとともに加圧されてなる正極層および負極層と、これら正極層および負極層の間に配置される固体電解質層とを具備する全固体二次電池であって、
上記正極層および負極層は、硫化物無機固体電解質を有し、
上記正極集電体および負極集電体は、ピール試験による硫化物無機固体電解質との剥離強度が0.2N/mm以上であることを特徴とする全固体二次電池。 - 固体電解質層は、硫化物無機固体電解質からなることを特徴とする請求項1に記載の全固体二次電池。
- 正極集電体は、錫またはエッチドアルミニウムであり、
負極集電体は、粗化銅であることを特徴とする請求項1または2に記載の全固体二次電池。
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KR1020167026394A KR102350322B1 (ko) | 2014-03-28 | 2015-03-26 | 전고체 2차전지 |
CN201580012833.2A CN106068577B (zh) | 2014-03-28 | 2015-03-26 | 全固态二次电池及其制造方法 |
EP15769914.1A EP3125351B1 (en) | 2014-03-28 | 2015-03-26 | All-solid-state secondary battery |
JP2016510462A JP6639383B2 (ja) | 2014-03-28 | 2015-03-26 | 全固体二次電池 |
US15/129,695 US20170179519A1 (en) | 2014-03-28 | 2015-03-26 | All-solid-state secondary battery |
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JP2014-067318 | 2014-03-28 | ||
JP2014067318 | 2014-03-28 |
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US (1) | US20170179519A1 (ja) |
EP (1) | EP3125351B1 (ja) |
JP (1) | JP6639383B2 (ja) |
KR (1) | KR102350322B1 (ja) |
CN (1) | CN106068577B (ja) |
WO (1) | WO2015147122A1 (ja) |
Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
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JP2017157271A (ja) * | 2016-02-29 | 2017-09-07 | 日立造船株式会社 | 全固体二次電池およびその製造方法 |
JP2017183121A (ja) * | 2016-03-31 | 2017-10-05 | 日立造船株式会社 | 全固体二次電池の製造方法 |
EP3425719A4 (en) * | 2016-02-29 | 2019-09-18 | Hitachi Zosen Corporation | FULLY SOLID RECHARGEABLE BATTERY AND METHOD FOR MANUFACTURING THE SAME |
US11145907B2 (en) * | 2017-03-28 | 2021-10-12 | Sanyo Electric Co., Ltd. | Method for producing secondary battery having negative electrode with different surface roughnesses |
US11476503B2 (en) | 2018-12-12 | 2022-10-18 | Panasonic Intellectual Property Management Co., Ltd. | All-solid-state battery |
Families Citing this family (3)
Publication number | Priority date | Publication date | Assignee | Title |
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US10446873B2 (en) * | 2016-12-30 | 2019-10-15 | Intel Corporation | Solid-state battery |
JP7100798B2 (ja) * | 2018-01-09 | 2022-07-14 | トヨタ自動車株式会社 | 非水電解液二次電池 |
KR20220132175A (ko) * | 2021-03-23 | 2022-09-30 | 주식회사 엘지에너지솔루션 | 습윤 상태의 전극 시편에 대한 접착력 측정 시스템 및 이를 이용한 습윤 상태의 전극 시편에 대한 접착력 측정 방법 |
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- 2015-03-26 KR KR1020167026394A patent/KR102350322B1/ko active IP Right Grant
- 2015-03-26 EP EP15769914.1A patent/EP3125351B1/en active Active
- 2015-03-26 US US15/129,695 patent/US20170179519A1/en not_active Abandoned
- 2015-03-26 JP JP2016510462A patent/JP6639383B2/ja active Active
- 2015-03-26 WO PCT/JP2015/059286 patent/WO2015147122A1/ja active Application Filing
- 2015-03-26 CN CN201580012833.2A patent/CN106068577B/zh active Active
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JP2017157271A (ja) * | 2016-02-29 | 2017-09-07 | 日立造船株式会社 | 全固体二次電池およびその製造方法 |
EP3425719A4 (en) * | 2016-02-29 | 2019-09-18 | Hitachi Zosen Corporation | FULLY SOLID RECHARGEABLE BATTERY AND METHOD FOR MANUFACTURING THE SAME |
US11101497B2 (en) | 2016-02-29 | 2021-08-24 | Hitachi Zosen Corporation | All-solid state secondary battery and method for manufacturing same |
JP2017183121A (ja) * | 2016-03-31 | 2017-10-05 | 日立造船株式会社 | 全固体二次電池の製造方法 |
US11145907B2 (en) * | 2017-03-28 | 2021-10-12 | Sanyo Electric Co., Ltd. | Method for producing secondary battery having negative electrode with different surface roughnesses |
US11476503B2 (en) | 2018-12-12 | 2022-10-18 | Panasonic Intellectual Property Management Co., Ltd. | All-solid-state battery |
Also Published As
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JPWO2015147122A1 (ja) | 2017-04-13 |
EP3125351A4 (en) | 2017-02-01 |
EP3125351B1 (en) | 2019-06-05 |
EP3125351A1 (en) | 2017-02-01 |
CN106068577B (zh) | 2019-09-24 |
CN106068577A (zh) | 2016-11-02 |
KR20160138967A (ko) | 2016-12-06 |
US20170179519A1 (en) | 2017-06-22 |
KR102350322B1 (ko) | 2022-01-11 |
JP6639383B2 (ja) | 2020-02-05 |
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