WO2015093590A1 - 電池の製造方法 - Google Patents
電池の製造方法 Download PDFInfo
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- WO2015093590A1 WO2015093590A1 PCT/JP2014/083663 JP2014083663W WO2015093590A1 WO 2015093590 A1 WO2015093590 A1 WO 2015093590A1 JP 2014083663 W JP2014083663 W JP 2014083663W WO 2015093590 A1 WO2015093590 A1 WO 2015093590A1
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- battery
- positive electrode
- sulfur
- oil
- active material
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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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/581—Chalcogenides or intercalation compounds thereof
- H01M4/5815—Sulfides
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B29B17/00—Recovery of plastics or other constituents of waste material containing plastics
- B29B17/02—Separating plastics from other materials
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10B—DESTRUCTIVE DISTILLATION OF CARBONACEOUS MATERIALS FOR PRODUCTION OF GAS, COKE, TAR, OR SIMILAR MATERIALS
- C10B53/00—Destructive distillation, specially adapted for particular solid raw materials or solid raw materials in special form
- C10B53/07—Destructive distillation, specially adapted for particular solid raw materials or solid raw materials in special form of solid raw materials consisting of synthetic polymeric materials, e.g. tyres
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/04—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of carbon-silicon compounds, carbon or silicon
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/20—Conductive material dispersed in non-conductive organic material
- H01B1/24—Conductive material dispersed in non-conductive organic material the conductive material comprising carbon-silicon compounds, carbon or silicon
-
- 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
- H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
-
- 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
- H01M4/1397—Processes of manufacture of electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
-
- 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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
-
- 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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
- H01M4/625—Carbon or graphite
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B29B17/00—Recovery of plastics or other constituents of waste material containing plastics
- B29B17/02—Separating plastics from other materials
- B29B2017/0213—Specific separating techniques
- B29B2017/0268—Separation of metals
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29L—INDEXING SCHEME ASSOCIATED WITH SUBCLASS B29C, RELATING TO PARTICULAR ARTICLES
- B29L2030/00—Pneumatic or solid tyres or parts thereof
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29L—INDEXING SCHEME ASSOCIATED WITH SUBCLASS B29C, RELATING TO PARTICULAR ARTICLES
- B29L2031/00—Other particular articles
- B29L2031/34—Electrical apparatus, e.g. sparking plugs or parts thereof
- B29L2031/3468—Batteries, accumulators or fuel cells
-
- 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 a method for producing a battery (a positive electrode active material, a positive electrode conductive material, a positive electrode current collector, and a negative electrode active material used for a battery) by using rubber containing sulfur such as a tire as a raw material.
- ⁇ Collected rubber is processed at a processing plant for recycling.
- a process of thermally decomposing rubbers using a pyrolysis furnace is performed (for example, see Patent Document 1).
- Rubbers were not effectively recycled as resources, only to the extent that recycled products that had been pyrolyzed at the above processing plant were used as heat sources.
- batteries such as lithium ion secondary batteries have attracted attention due to the spread of electric products and the development of electric vehicles, and in particular, it is desired to increase the capacity of the batteries.
- the present inventor conducted extensive research on a method for effectively reusing and recycling sulfur-containing rubbers such as tires that are discharged in large quantities as a battery.
- the raw material in a battery manufacturing method for manufacturing a battery using sulfur-containing rubbers such as tires as a raw material, the raw material is pyrolyzed and separated into a solid and a dry distillation gas, The dry distillation gas is cooled and separated into oil and gas, the oil is distilled and separated into heavy oil, light oil and sulfur, and the heavy oil and sulfur are kneaded and heat treated to produce a positive electrode active material. Decided to do.
- a battery manufacturing method for manufacturing a battery by using rubber containing sulfur such as tire as a raw material rubber containing sulfur such as tire is used as a raw material. Pyrolysis separates into solid and dry distillation gas, cools the dry distillation gas to separate into oil and gas, distills the oil to separate into heavy oil, light oil and sulfur, heavy oil
- the positive electrode active material of the battery is manufactured by kneading and heat-treating, and the solid material is sorted into metal and carbide, and the positive electrode conductive material of the battery is manufactured by heat-treating the carbide. And a positive electrode current collector of the battery using the positive electrode conductive material.
- a raw material in the manufacturing method of the battery which manufactures a battery using rubber
- the solid material was classified into metal and carbide, and the positive electrode conductive material for the battery was manufactured by heat treating the carbide.
- the raw material in a battery manufacturing method for manufacturing a battery using sulfur-containing rubbers such as tires as a raw material, the raw material is pyrolyzed and separated into a solid and a dry distillation gas.
- the solid material was sorted into metal and carbide, and the carbide was heat-treated to produce a negative electrode active material body for the battery.
- rubbers containing sulfur such as tires discharged in large quantities can be effectively recycled as batteries.
- Process drawing which shows process of rubber
- Explanatory drawing which shows the charging / discharging characteristic of a battery.
- Explanatory drawing which shows the charging / discharging characteristic of a battery.
- Explanatory drawing which shows the charging / discharging characteristic of a battery.
- the present invention uses a rubber as a raw material to produce a positive electrode active material, a positive electrode conductive material and a negative electrode active material used in a battery, and also uses a positive electrode active material and a positive electrode conductive material.
- rubbers include rubber products containing various sulfur and silicon such as tires discarded after use, and rubbers containing sulfur and silicon that are generated and discarded as defective products or surplus materials in the manufacturing process. It is possible to use a waste mainly composed of.
- the raw rubbers are pyrolyzed using a pyrolysis furnace. Thereby, it isolate
- Solid matter separated from rubber by thermal decomposition is subjected to a sorting process using a sorter. Thereby, it sorts into a metal and carbide.
- Metals selected from solids can be recycled as metal resources.
- the carbide selected from solids is pulverized using a pulverizer and then heat-treated (2400 ° C to 2800 ° C) using a heat treatment machine to remove the contained zinc, thereby forming a hollow highly conductive material. be able to. It can be recycled as it is as the positive electrode conductive material of the battery. Moreover, after removing the iron contained by further washing, it can be recycled as the positive electrode conductive material of the battery.
- This carbide can be used as an active material for a capacitor or a carrier material for a fuel cell catalyst by activating carbonization after pulverization, or by activating carbonization after heat treatment after pulverization. Further, the carbide can be pulverized and recycled as a negative electrode active material for a battery, and the negative electrode active material can be recycled as a negative electrode current collector for a battery by molding the negative electrode active material with a binder.
- the dry distillation gas separated from rubber by thermal decomposition is cooled using a cooler. Thereby, it isolate
- the production ratio and components of heavy oil and non-condensable gas can be controlled by the cooling temperature of the cooler.
- the cooling temperature When the cooling temperature is lowered, the production ratio of heavy oil increases and the amount of hydrocarbons contained in the non-condensed gas decreases. Therefore, the hydrocarbon concentration of the non-condensable gas can be detected by a detector, and the cooling temperature can be controlled so that the concentration becomes constant.
- the non-condensed gas separated from the dry distillation gas is depressurized using a safety device and then desulfurized using a desulfurizer.
- the hydrocarbon gas which does not contain sulfur content from non-condensable gas is recoverable.
- the recovered hydrocarbon gas may be recovered for each gas component using a fractionator or the like.
- the hydrocarbon gas recovered in this way does not contain sulfur and contains a large amount of carbon, so that it can be effectively used as a raw material for carbon nanotubes, carbon nanofibers, and the like.
- the sulfur recovered by the desulfurizer can be effectively used for the production of the positive electrode active material described later.
- the oil separated from the dry distillation gas is distilled using a distiller at a temperature above the boiling point of sulfur.
- a distiller at a temperature above the boiling point of sulfur.
- Light oil containing sulfur is recovered by separating it into sulfur and light oil by desulfurization treatment.
- the separated light oil can be recycled as fuel.
- the separated heavy oil and sulfur can be kneaded using a kneader and heat treated (reflux heat treatment or autoclave treatment) using a heat treatment machine to produce a solid positive electrode active material.
- the sulfur used for the production of the positive electrode active material is not limited to rubbers extracted from heavy oil, but those produced from other raw materials or commercially available products may be used, or a mixture thereof. But you can.
- rubbers containing sulfur such as tires are used as raw materials, the raw materials are pyrolyzed and separated into solids and dry distillation gas, the dry distillation gas is cooled and separated into oil and gas components,
- a positive electrode active material for a battery can be produced by distilling the oil to separate it into heavy oil, light oil and sulfur, and kneading and heat treating the heavy oil and sulfur.
- the positive electrode active material thus manufactured was pulverized, mixed with a conductive material, a binder and a solvent and molded to produce a battery (positive electrode current collector).
- the same thing as the lithium ion secondary battery using the existing cobalt as an active material was used for the electrically conductive material, the binder, and the solvent in the same ratio.
- the capacity per weight was about 200 mAh / g, whereas in the battery according to the present invention, as shown in FIG. 2, 400 mAh / g. Capacities exceeding the capacity could be manufactured.
- FIG. 2 shows the charge / discharge characteristics of the battery according to the present invention.
- the battery was repeatedly charged / discharged at a discharge end voltage of 1.0 V and a charge end voltage of 3.0 V at a current of 50 mA per 1 g of the positive electrode active material. It is. In the initial discharge, the capacity exceeds 900 mAh / g, and the capacity exceeds 400 mAh / g even after 11 charge / discharge cycles.
- the positive electrode active material according to the present invention can increase the capacity of the battery.
- rubber containing sulfur such as tire is used as a raw material, the raw material is pyrolyzed and separated into solid and dry distillation gas, the solid is sorted into metal and carbide, and the carbide is heat treated.
- the positive electrode conductive material of the battery can be manufactured.
- a battery (positive electrode current collector) was manufactured by mixing the positive electrode conductive material manufactured in this way with the positive electrode active material according to the present invention, a binder, and a solvent and molding the mixture.
- the same thing as the lithium ion secondary battery using the existing cobalt as an active material was used for the binder and the solvent in the same ratio.
- the same positive electrode active material as above was used in the same ratio.
- the capacity per weight in the initial discharge exceeded 900 mAh / g, whereas As shown in FIG.
- FIG. 3 shows the charge / discharge characteristics of the battery according to the present invention
- the dotted line shows the characteristics of the lithium ion secondary battery using the positive electrode active material according to the present invention and the existing conductive material (similar to FIG. 2).
- the solid line shows the characteristics of the lithium ion secondary battery using the positive electrode active material and the positive electrode conductive material according to the present invention.
- the end-of-discharge voltage of 1. mA is obtained at a current of 50 mA per 1 g of the positive electrode active material.
- the battery is charged and discharged at 0 V and a charge end voltage of 3.0 V.
- the initial capacity of the battery can be increased.
- rubber containing sulfur such as tires is used as a raw material, the raw material is pyrolyzed and separated into solid and dry distillation gas, the solid is sorted into metal and carbide, and the carbide is heat treated.
- the negative electrode active material of a battery can be manufactured.
- the battery (negative electrode current collector) was manufactured by pulverizing the negative electrode active material thus manufactured, mixing it with a binder and molding it.
- the binder was used at the same ratio as the lithium ion secondary battery using existing graphite as an active material.
- the capacity per weight was about 360 mAh / g, whereas in the battery according to the present invention, as shown in FIG. 4, 900 mAh / g. Capacities exceeding the capacity could be manufactured.
- FIG. 4 shows the charge / discharge characteristics of the battery according to the present invention.
- Charge / discharge was repeatedly performed at a discharge end voltage of 0.03 V and a charge end voltage of 1.5 V at a current of 50 mA per 1 g of the negative electrode current collector. Is. In the initial discharge, the capacity exceeds 1200 mAh / g, and the capacity exceeds 900 mAh / g even after repeated charging and discharging five times.
- the capacity of the battery can be increased.
- rubber containing sulfur such as tires is used as a raw material, the raw material is pyrolyzed to separate into solid and dry distillation gas, and the dry distillation gas is cooled to obtain oil and gas.
- the oil component is distilled to separate heavy oil, light oil and sulfur, and the positive electrode active material of the battery is manufactured by kneading and heat treating the heavy oil and sulfur.
- the positive electrode active material and the negative electrode active material of the battery are manufactured by sorting the carbide into carbides and heat-treating the carbide, and the positive electrode current collector of the battery is manufactured using the positive electrode active material and the positive electrode conductive material.
- a positive electrode current collector or a negative electrode current collector can be used to manufacture a battery.
- the positive electrode active material, the positive electrode conductive material, the positive electrode current collector, the negative electrode active material, and the negative electrode current collector according to the present invention are not limited to the case where the same battery is manufactured from them, and the case where each battery is manufactured separately. It can also be used.
- rubber containing sulfur such as tires discharged in large quantities can be effectively recycled as a battery.
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Abstract
Description
Claims (4)
- タイヤ等の硫黄を含有するゴム類を原料に用いて電池を製造する電池の製造方法において、
原料を熱分解して固形物と乾留ガスとに分離し、前記乾留ガスを冷却して油分とガスとに分離し、油分を蒸留して重質油と軽質油と硫黄とに分離し、重質油と硫黄とを混練し熱処理することで正極活物質を製造することを特徴とする電池の製造方法。 - タイヤ等の硫黄を含有するゴム類を原料に用いて電池を製造する電池の製造方法において、
タイヤ等の硫黄を含有するゴム類を原料とし、原料を熱分解して固形物と乾留ガスとに分離し、
前記乾留ガスを冷却して油分とガスとに分離し、油分を蒸留して重質油と軽質油と硫黄とに分離し、重質油と硫黄とを混練し熱処理することで電池の正極活物質を製造し、
前記固形物を金属と炭化物とに選別し、炭化物を熱処理することで電池の正極導電材を製造し、
前記正極活物質と前記正極導電材とを用いて電池の正極集電体を製造することを特徴とする電池の製造方法。 - タイヤ等の硫黄を含有するゴム類を原料に用いて電池を製造する電池の製造方法において、
原料を熱分解して固形物と乾留ガスとに分離し、前記固形物を金属と炭化物とに選別し、炭化物を熱処理することで電池の正極導電材を製造することを特徴とする電池の製造方法。 - タイヤ等の硫黄を含有するゴム類を原料に用いて電池を製造する電池の製造方法において、
原料を熱分解して固形物と乾留ガスとに分離し、前記固形物を金属と炭化物とに選別し、炭化物を熱処理することで電池の負極活物質を製造することを特徴とする電池の製造方法。
Priority Applications (8)
Application Number | Priority Date | Filing Date | Title |
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JP2015553617A JP6266655B2 (ja) | 2013-12-20 | 2014-12-19 | 電池の製造方法 |
CA2937220A CA2937220C (en) | 2013-12-20 | 2014-12-19 | Battery production method |
ES14872552T ES2779063T3 (es) | 2013-12-20 | 2014-12-19 | Método de fabricación de batería |
KR1020167015610A KR101750333B1 (ko) | 2013-12-20 | 2014-12-19 | 전지의 제조방법 |
EP14872552.6A EP3086391B1 (en) | 2013-12-20 | 2014-12-19 | Battery production method |
DK14872552.6T DK3086391T3 (da) | 2013-12-20 | 2014-12-19 | Batterifremstillingsfremgangsmåde |
CN201480069320.0A CN105830262B (zh) | 2013-12-20 | 2014-12-19 | 电池的制造方法 |
US15/184,204 US9991516B2 (en) | 2013-12-20 | 2016-06-16 | Battery production method |
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JP2013-263200 | 2013-12-20 | ||
JP2013263200 | 2013-12-20 |
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US15/184,204 Continuation US9991516B2 (en) | 2013-12-20 | 2016-06-16 | Battery production method |
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WO2015093590A1 true WO2015093590A1 (ja) | 2015-06-25 |
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US (1) | US9991516B2 (ja) |
EP (1) | EP3086391B1 (ja) |
JP (1) | JP6266655B2 (ja) |
KR (1) | KR101750333B1 (ja) |
CN (1) | CN105830262B (ja) |
CA (1) | CA2937220C (ja) |
DK (1) | DK3086391T3 (ja) |
ES (1) | ES2779063T3 (ja) |
PT (1) | PT3086391T (ja) |
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Cited By (1)
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WO2024085192A1 (ja) * | 2022-10-18 | 2024-04-25 | 株式会社ルネシス | 電極部材の製造方法及び電極部材の製造システム、並びに正極活物質の製造方法、正極活物質、正極合剤及び二次電池 |
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JP5400064B2 (ja) * | 2008-12-26 | 2014-01-29 | Jx日鉱日石エネルギー株式会社 | リチウムイオン二次電池負極材料用の原料油組成物 |
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- 2014-12-19 ES ES14872552T patent/ES2779063T3/es active Active
- 2014-12-19 JP JP2015553617A patent/JP6266655B2/ja active Active
- 2014-12-19 CA CA2937220A patent/CA2937220C/en active Active
- 2014-12-19 CN CN201480069320.0A patent/CN105830262B/zh active Active
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO2024085192A1 (ja) * | 2022-10-18 | 2024-04-25 | 株式会社ルネシス | 電極部材の製造方法及び電極部材の製造システム、並びに正極活物質の製造方法、正極活物質、正極合剤及び二次電池 |
JP7485439B1 (ja) | 2022-10-18 | 2024-05-16 | 株式会社ルネシス | 電極部材の製造方法及び電極部材の製造システム、並びに正極活物質の製造方法、正極活物質、正極合剤及び二次電池 |
Also Published As
Publication number | Publication date |
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CN105830262B (zh) | 2018-05-29 |
CA2937220A1 (en) | 2015-06-25 |
KR20160085869A (ko) | 2016-07-18 |
DK3086391T3 (da) | 2020-04-06 |
EP3086391A4 (en) | 2017-09-06 |
EP3086391B1 (en) | 2020-01-22 |
JP6266655B2 (ja) | 2018-01-24 |
US20160359167A1 (en) | 2016-12-08 |
KR101750333B1 (ko) | 2017-06-23 |
ES2779063T3 (es) | 2020-08-13 |
CA2937220C (en) | 2020-06-09 |
EP3086391A1 (en) | 2016-10-26 |
CN105830262A (zh) | 2016-08-03 |
US9991516B2 (en) | 2018-06-05 |
PT3086391T (pt) | 2020-03-13 |
JPWO2015093590A1 (ja) | 2017-03-23 |
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