WO2015056417A1 - 制御弁式鉛蓄電池 - Google Patents
制御弁式鉛蓄電池 Download PDFInfo
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- WO2015056417A1 WO2015056417A1 PCT/JP2014/005048 JP2014005048W WO2015056417A1 WO 2015056417 A1 WO2015056417 A1 WO 2015056417A1 JP 2014005048 W JP2014005048 W JP 2014005048W WO 2015056417 A1 WO2015056417 A1 WO 2015056417A1
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- WIPO (PCT)
- Prior art keywords
- current collector
- positive electrode
- acid battery
- lead
- average layer
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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
- H01M10/06—Lead-acid accumulators
- H01M10/12—Construction or manufacture
- H01M10/121—Valve regulated lead acid batteries [VRLA]
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C11/00—Alloys based on lead
- C22C11/06—Alloys based on lead with tin as the next major constituent
-
- 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
- H01M10/06—Lead-acid accumulators
-
- 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
- H01M4/68—Selection of materials for use in lead-acid accumulators
- H01M4/685—Lead alloys
-
- 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
- H01M4/70—Carriers or collectors characterised by shape or form
- H01M4/72—Grids
- H01M4/73—Grids for lead-acid accumulators, e.g. frame plates
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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
- H01M10/06—Lead-acid accumulators
- H01M10/08—Selection of materials as electrolytes
- H01M10/10—Immobilising of electrolyte
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2220/00—Batteries for particular applications
- H01M2220/10—Batteries in stationary systems, e.g. emergency power source in plant
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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
Definitions
- This invention relates to a control valve type lead acid battery, and more particularly to its positive electrode grid.
- a cast grid is generally used for the positive current collector of a control valve type lead-acid battery (hereinafter sometimes referred to as “VRLA battery”) used for emergency power supply (UPS) in hospitals and factories. Is never used.
- VRLA battery for stationary use is always float-charged and maintained in a fully charged state, and therefore, it is general that lattice corrosion of the positive electrode becomes a life mode.
- a certain thickness is required for the pole of the positive grid, but in the case of an expanded grid, it is difficult to create a thick grid, which is not suitable for a large stationary VRLA battery.
- the expanded lattice when used as the positive electrode lattice of the VRLA battery, the positive electrode corrosion current during charging is large and the float current is not used for oxygen generation, so that the oxygen absorption cycle in the negative electrode plate becomes incomplete.
- the negative electrode When the oxygen absorption cycle becomes incomplete, the negative electrode is polarized. As a result, the float current decreases, the positive electrode becomes insufficiently charged, and the discharge capacity decreases.
- the expanded grid is used for the positive electrode of the VRLA battery used in this way, the float current becomes small and the life becomes short due to insufficient charging. Therefore, a cast grid has been used for the control valve type lead-acid battery.
- Patent Document 1 JP2006-294296A discloses that rolling is performed at a small reduction rate in the initial stage of rolling to maintain the strength of the deep layer portion of the rolled sheet.
- Patent Document 2 JP2008-84676A states that intergranular corrosion is suppressed when the average particle size along the rolling direction is 150 ⁇ m or less with respect to the expanded lattice (positive electrode lattice) of the lead storage battery.
- Patent Document 3 JP2000-348758A discloses a VRLA battery using an expanded lattice as a positive electrode lattice.
- the inventor has focused on the fact that when the cast current collector is a positive electrode current collector of a VRLA battery, intergranular corrosion proceeds, so that the strength of the positive electrode current collector is significantly reduced at the end of the life.
- the strength of the positive electrode current collector is reduced, there arises a problem that the positive electrode grid collapses or breaks at the time of disasters such as vibration and earthquake, and the necessary discharge performance cannot be obtained.
- An object of the present invention is to provide a control valve type lead-acid battery that has a long life and is excellent in earthquake resistance even at the end of its life.
- the present invention relates to a control valve type lead storage battery having a positive electrode current collector, a positive electrode active material, a negative electrode current collector, a negative electrode active material, and a liquid retaining material, wherein the positive electrode current collector punches a rolled sheet of a lead alloy. Further, the punched current collector is characterized in that the average layer spacing of the layered current collector structure in the cross section in the thickness direction of the current collector is 25 ⁇ m or more and 180 ⁇ m or less.
- the positive electrode current collector is formed by punching a rolled sheet of a lead alloy.
- the punched current collector is characterized in that the average layer spacing of the layered lattice structure is 25 ⁇ m or more and 180 ⁇ m or less in the cross section in the thickness direction of the current collector parallel to the rolling direction.
- the inventor has found that the float life and the earthquake resistance at the end of the life depend on the average layer spacing of the rolled structure of the positive electrode current collector. That is, when the average layer interval is reduced, the float life is shortened, and particularly when the average layer distance is less than 25 ⁇ m, the life is shortened. This is because, in a positive grid having a small average layer spacing, the corrosion mechanism is mainly lamellar corrosion, and the smaller the average layer spacing, the faster the layered corrosion proceeds. The float life varies significantly depending on whether the average layer spacing is 25 ⁇ m or more.
- the effect of intergranular corrosion differs depending on whether the average layer spacing is 180 ⁇ m or less, and if the average layer spacing is 180 ⁇ m or less, the earthquake resistance at the end of life is improved.
- the cast slab When the cast slab is rolled, it changes from a cast structure having a large number of crystal grains to a layered structure.
- the average layer spacing is 180 ⁇ m or less, there are almost no crystal grain boundaries, and the corrosion progresses in layers, so that the intergranular corrosion does not occur. This is because there is no breakage.
- the average layer spacing is 50 ⁇ m or more, the float life is further improved, and when it is 150 ⁇ m or less, the earthquake resistance at the end of the life is further improved. Therefore, the average layer spacing is particularly preferably 50 ⁇ m or more and 150 ⁇ m or less.
- the rate of intergranular corrosion is determined by the crystal grain size and the number of crystal grains. It is also known that intergranular corrosion does not occur in a layered rolled structure. In addition to these, it has been found that the average interlayer spacing affects the rate of laminar corrosion. For this reason, in the case of a positive electrode current collector by rolling, if the composition is the same, it is the average layer spacing that affects the float life and the earthquake resistance at the end of the life. And the influence of the particle diameter along the rolling direction on these performances is small. As shown in FIG. 5, the average layer spacing is related to the rolling reduction, and the preferable rolling reduction range is 60% or more and 90% or less.
- the positive electrode current collector is made of a Pb—Ca—Sn alloy, and in mass% units, when the Ca content is x and the Sn content is y, 0.03 ⁇ x ⁇ 0.09, 9.16x + 0.525 ⁇ y ⁇ 2.0.
- This composition range is shown in the hatched frame in FIG. 2, and the float life is reduced even if it deviates from this range to any side. This can be confirmed from Examples 1 to 7 and Examples 25 to 28 in Table 3 (both average layer spacing is 62 ⁇ m).
- the positive electrode lattice may contain an antioxidant and inevitable impurities in a total amount of 0.04 mass% or less.
- the punched current collector has a frame around the four circumferences of the grid. Therefore, the charge / discharge current is made uniform over the entire grid, and the capacity reduction due to insufficient charging is unlikely to proceed.
- the average layer spacing can be measured by observing the cross section of the positive electrode current collector with a metal microscope, for example, at the ear and the frame bone.
- the layer spacing can be observed regardless of the rolling direction, but is easier to measure when observed in the rolling direction.
- the edge of the positive electrode current collector is cut in the vertical direction and the horizontal direction (both perpendicular to the thickness direction), the cut surface is observed with a metal microscope, and the crystal grain size increases in the rolling direction.
- observe three cross-sections at the ears of the positive electrode current collector and three cross-sections at the current collector frame and use the ratio between the thickness of the current collector and the number of layers as the layer spacing.
- the average value of the six locations is taken as the average layer spacing.
- FIG. 4 is a diagram showing how to obtain the average layer spacing.
- the cross section of the current collector with a thickness of 0.8 mm is observed, and as shown by the red line, there are 13 layers.
- the layer spacing is 62 ⁇ m.
- the rolling direction refers to the traveling direction when a slab, which is a lump of lead alloy, passes through a rolling device such as a roll to form a sheet.
- a method of punching the current collector in the direction shown in FIG. 6B there are a method of punching the current collector in the direction shown in FIG. 6B and a method of punching in a different direction. The punching may be performed in any direction.
- Current collectors include grid-shaped current collectors commonly referred to as grids, current collectors punched out of circles and ellipses, and grids that are provided radially from the ears of the current collectors. Even if it is a thing, a collector may only be called a grating
- the current collector is simply referred to as a lattice.
- the punched grid 2 is shown in FIG. 1 (a), and the expanded grid 10 is shown in FIG. 1 (b) for comparison.
- 4 is an ear
- 5 and 6 are frames
- 7 is a foot.
- the expanded lattice 10 does not have a frame 6. Since the punched grid 2 has the frame 6, the elongation of the grid due to corrosion is suppressed, and the entire positive electrode plate is easily charged and discharged uniformly.
- Pb—Ca—Sn alloy sheets having compositions 1 to 11 were prepared.
- Rolled sheets having an average layer spacing of 14 ⁇ m, 26 ⁇ m, 62 ⁇ m, 125 ⁇ m, 178 ⁇ m, and 199 ⁇ m were produced cold while changing the rolling reduction.
- the rolled sheet was punched into a positive grid with a thickness of 3 mm.
- an expanded grid was manufactured from a rolled sheet having an average layer spacing of 62 ⁇ m, and a positive grid was manufactured by casting.
- the rolling reduction was adjusted according to the lattice composition, and the rolling average was changed to the required average layer spacing.
- Table 2 shows the average layer spacing of the rolled structure for a typical positive electrode lattice.
- the rolling reduction is how much the thickness of the slab, which is a lump of lead alloy, changes when the slab before rolling is turned into a sheet when it passes through a rolling device such as a roll. Good, (Slab thickness ⁇ sheet thickness) / slab thickness ⁇ 100 (%).
- As an unformed positive electrode active material 99.9 mass% of lead powder by ball mill method and 0.1 mass% of synthetic resin fiber are pasted with sulfuric acid with a specific gravity of 1.16 at 25 ° C, filled into the positive electrode lattice, dried and aged. They were connected to each other with a strap to form an electrode plate group consisting of four positive electrode plates.
- the composition and density of the positive electrode active material are arbitrary.
- a negative electrode lattice containing 0.1 mass% Ca, 0.7 mass% Sn, 0.02 mass% Al, and the balance being Pb and inevitable impurities was cast.
- the composition of the negative electrode lattice, the type of lattice such as casting and punching, and parameters such as the average layer spacing are arbitrary.
- As an anode active material a lead powder 98.3Mass% of ball mill method, the synthetic resin fibers 0.1mass%, carbon black 0.1mass%, BaSO 4 1.4mass%, and a lignin 0.1mass%, in the specific gravity of 1.14 at 25 ° C. sulfate It was pasted and filled into the negative electrode grid. After drying and aging, they were connected to each other with a strap to form an electrode plate group consisting of five negative electrode plates.
- a retainer liquid such as a retainer mat is placed between the positive electrode plate and the negative electrode plate, accommodated in the battery case while applying pressure, sulfuric acid is added as the electrolyte, and the battery case is formed, and the capacity is 60 Ah. It was set as the control valve type lead acid battery. Silica gel or the like may be used as the liquid retaining liquid, and the configuration of the control valve type lead storage battery is arbitrary except for the positive grid. For example, the negative grid can be cast, expanded, or stamped. The composition of the positive electrode active material and the negative electrode active material is arbitrary.
- the casting grid (Comparative Examples 1 to 3) has a long float life, but has a low capacity retention rate at the end of the lifetime, which is due to the collapse of the grid due to intergranular corrosion and the loss of the positive electrode active material.
- the expanded lattice (Comparative Examples 4 to 6) had an extremely short float life, and in particular, the float life was significantly shorter than the punched lattice (Examples 2, 5 and 6) having the same lattice composition and the same average layer spacing. This means that the corrosion current increased due to the use of a rolled sheet for the grid, and that the current distribution became non-uniform because there was no grid vertical frame, resulting in insufficient charging and an early decrease in discharge capacity. Show.
- composition 8-11 (Examples 25 to 32) out of the optimal range had a short float life.
- the strength of the lattice is low from the beginning, and when it exceeds 0.09 mass%, the corrosion is likely to proceed. It was also found that corrosion tends to proceed when the Sn concentration deviates from the optimum range.
- the VRLA batteries of Examples 25 to 32 are included in the present invention in that both the float life performance and the earthquake resistance at the end of the life are compatible by optimizing the average layer spacing.
- VRLA battery for stationary use
- a charging method other than float charging may be used, and it may be used for purposes other than stationary use.
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Abstract
Description
好ましくは、正極集電体と正極活物質と、負極集電体と負極活物質と、保液体とを有する制御弁式鉛蓄電池において、前記正極集電体は、鉛合金の圧延シートを打ち抜いた打抜き集電体で、圧延方向に平行でかつ集電体の厚さ方向の断面での、層状の格子組織の平均層間隔が25μm以上180μm以下であることを特徴とする。
層間隔が25μm以上か未満かで、フロート寿命は著しく異なる。
図4は、平均層間隔の求め方を示した図であり、0.8 mmの厚さの集電体の断面を観察し、赤線で示したように、層が13層あるため、平均層間隔は62μmとなる。
尚、圧延方向とは、鉛合金の塊であるスラブが、ロールなどの圧延装置を通過してシートとされた時の進行方向をいう。
圧延シートから集電体を作製する際には、集電体の耳部を図6(b)に示す方向に向けてシートから打抜く方法と、それとは別の方向で打抜く方法とがあり、どのような方向で打抜きを行ってもよい。
集電体とは、一般にグリッドと呼ばれる格子状の集電体や、円や楕円を打抜いた集電体、集電体の耳部から放射状にグリッドを設けたものなどがあり、格子状でないものであっても、単に集電体を格子と呼ぶ場合もある。
以降、実施例では、集電体を単に格子と呼ぶ。
圧下率とは、鉛合金の塊であるスラブが、ロールなどの圧延装置を通過してシートとされた時の、圧延を行う前のスラブがシートになった時に厚みがどれだけ変化したかをいい、
(スラブ厚-シート厚み)/スラブ厚×100(%)で示される。
4 耳部
5,6 枠
7 足
8,12 桟
10 エキスパンド格子
Claims (10)
- 正極集電体と正極活物質と、負極集電体と負極活物質と、保液体とを有する制御弁式鉛蓄電池において、
前記正極集電体は、鉛合金の圧延シートを打ち抜いた打抜き集電体で、
集電体の厚さ方向の断面での、層状の集電体組織の平均層間隔が25μm以上180μm以下であることを特徴とする、制御弁式鉛蓄電池。 - 正極集電体と正極活物質と、負極集電体と負極活物質と、保液体とを有する制御弁式鉛蓄電池において、
前記正極集電体は、鉛合金の圧延シートを打ち抜いた打抜き集電体で、圧延方向に平行でかつ集電体の厚さ方向の断面での、層状の集電体組織の平均層間隔が25μm以上180μm以下であることを特徴とする、制御弁式鉛蓄電池。 - 前記正極集電体は、Pb-Ca-Sn合金から成り、mass%単位で、Ca含有量をx,Sn含有量をyとした際に、 0.03≦x≦0.09, 9.16x+0.525≦y≦2.0 であることを特徴とする、請求項1の制御弁式鉛蓄電池。
- 前記正極集電体は、桟の断面が長方形で、かつ4周に枠を備えていることを特徴とする、請求項1または2の制御弁式鉛蓄電池。
- 前記層状の集電体組織の平均層間隔が50μm以上180μm以下であることを特徴とする、請求項1~4のいずれかに記載の制御弁式鉛蓄電池。
- 前記層状の集電体組織の平均層間隔が25μm以上150μm以下であることを特徴とする、請求項1~4のいずれかに記載の制御弁式鉛蓄電池。
- 前記層状の集電体組織の平均層間隔が50μm以上150μm以下であることを特徴とする、請求項1~4のいずれかに記載の制御弁式鉛蓄電池。
- 病院や工場等の非常用電源装置、小型UPSなどの据置用途に用いられることを特徴とする請求項1~7に記載の制御弁式鉛蓄電池。
- 鉛合金の圧延シートを打ち抜いた打抜き集電体で、圧延方向に平行でかつ集電体の厚さ方向の断面での、層状の集電体組織の平均層間隔が25μm以上180μm以下である前記正極集電体と正極活物質と、負極集電体と負極活物質と、補液体とを用いた制御弁式鉛蓄電池の製造方法。
- 圧下率が60~90%となるように作製した鉛合金の圧延シートを打ち抜いた打抜き集電体で、圧延方向に平行でかつ集電体の厚さ方向の断面での、層状の集電体組織の平均層間隔が25μm以上180μm以下である前記正極集電体と正極活物質と、負極集電体と負極活物質と、補液体とを用いた制御弁式鉛蓄電池の製造方法。
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JP2015542514A JP6504055B2 (ja) | 2013-10-15 | 2014-10-03 | 制御弁式鉛蓄電池 |
US15/028,904 US10084209B2 (en) | 2013-10-15 | 2014-10-03 | Valve regulated lead-acid battery |
CN201480056581.9A CN105917503B (zh) | 2013-10-15 | 2014-10-03 | 阀控式铅蓄电池 |
EP14854597.3A EP3059791B1 (en) | 2013-10-15 | 2014-10-03 | Valve-regulated lead-acid battery |
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JP2013214836 | 2013-10-15 | ||
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JP2017139215A (ja) * | 2016-02-02 | 2017-08-10 | 株式会社Gsユアサ | 鉛蓄電池用の正極板、鉛蓄電池、鉛蓄電池用の正極板の製造方法 |
WO2020080422A1 (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池、および、鉛蓄電池の製造方法 |
WO2020080418A1 (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池およびその製造方法 |
WO2020080424A1 (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池用集電体およびその製造方法 |
JP2020064736A (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池用集電体、鉛蓄電池、および、鉛蓄電池用集電体の製造方法 |
WO2020080420A1 (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池 |
WO2020080421A1 (ja) | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池 |
WO2020080419A1 (ja) * | 2018-10-16 | 2020-04-23 | 株式会社Gsユアサ | 鉛蓄電池 |
JP2021163676A (ja) * | 2020-04-01 | 2021-10-11 | 古河電池株式会社 | 液式鉛蓄電池 |
WO2021210244A1 (ja) * | 2020-04-14 | 2021-10-21 | 株式会社Gsユアサ | 鉛蓄電池用集電体、鉛蓄電池用正極板、および鉛蓄電池 |
WO2022030416A1 (ja) * | 2020-08-05 | 2022-02-10 | 古河電気工業株式会社 | 鉛合金、鉛蓄電池用正極、鉛蓄電池、及び蓄電システム |
US11735742B2 (en) | 2019-05-31 | 2023-08-22 | Gs Yuasa International Ltd. | Lead-acid battery |
JP7385766B1 (ja) | 2022-09-09 | 2023-11-22 | 古河電池株式会社 | 鉛蓄電池用集電板、鉛蓄電池 |
US11894560B2 (en) | 2019-09-27 | 2024-02-06 | Gs Yuasa International Ltd. | Lead-acid battery |
JP7463719B2 (ja) | 2019-12-25 | 2024-04-09 | 株式会社Gsユアサ | 蓄電池用集電体および電極板 |
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US20160254570A1 (en) | 2016-09-01 |
JP6504055B2 (ja) | 2019-04-24 |
JP6835125B2 (ja) | 2021-02-24 |
EP3059791A1 (en) | 2016-08-24 |
CN105917503A (zh) | 2016-08-31 |
CN105917503B (zh) | 2019-03-29 |
EP3059791B1 (en) | 2021-12-29 |
EP3059791A4 (en) | 2017-06-21 |
US10084209B2 (en) | 2018-09-25 |
JP2019117802A (ja) | 2019-07-18 |
JPWO2015056417A1 (ja) | 2017-03-09 |
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