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WO2018061457A1 - Pile rechargeable au lithium-ion - Google Patents

Pile rechargeable au lithium-ion Download PDF

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Publication number
WO2018061457A1
WO2018061457A1 PCT/JP2017/027607 JP2017027607W WO2018061457A1 WO 2018061457 A1 WO2018061457 A1 WO 2018061457A1 JP 2017027607 W JP2017027607 W JP 2017027607W WO 2018061457 A1 WO2018061457 A1 WO 2018061457A1
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WO
WIPO (PCT)
Prior art keywords
water
binder
soluble
active material
thickener
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2017/027607
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English (en)
Japanese (ja)
Inventor
栄二 關
尚貴 木村
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Hitachi Astemo Ltd
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Hitachi Automotive Systems Ltd
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Filing date
Publication date
Application filed by Hitachi Automotive Systems Ltd filed Critical Hitachi Automotive Systems Ltd
Publication of WO2018061457A1 publication Critical patent/WO2018061457A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • 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
    • H01M10/0566—Liquid 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
    • H01M10/0566—Liquid materials
    • H01M10/0567—Liquid materials characterised by the additives
    • 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
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • 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
    • H01M10/0566—Liquid materials
    • H01M10/0569—Liquid materials characterised by the solvents
    • 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
    • H01M4/134—Electrodes based on metals, Si or 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
    • H01M4/13—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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • 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

Definitions

  • the present invention relates to an increase in capacity of a lithium ion secondary battery and electrode production.
  • An active material containing Si is expected as a negative electrode active material that can be expected to have a high energy density.
  • Si has a large volume change due to charge and discharge, the conductive network between the active material particles is destroyed, so that there is a disadvantage that cycle deterioration is large. Therefore, in patent document 1, the capacity
  • polyamide, polyimide, and polyamideimide as a binder to suppress expansion and contraction and improve cycle life.
  • the binder used is an organic solvent such as NMP.
  • equipment such as an exhaust duct is required, which increases the cost.
  • water-soluble polyamides that are soluble in water have been studied, and cost reduction can be expected.
  • the surface tension is larger than that of the organic solvent (for example, NMP), and the binder is aggregated at the time of producing the electrode, and the negative electrode mixture layer is easily peeled off, so there is room for improvement.
  • the object of the present invention is to have a water-soluble polyimide-based material or a water-soluble polyamide-based material as a binder, and a water-soluble thickener to suppress peeling at the time of electrode preparation. It is providing the lithium ion secondary battery which can reduce the cost of the electrode using this.
  • a first aspect of the present invention is a secondary battery having a negative electrode mainly composed of an Si-based active material as an active material, wherein the active material layer is a water-soluble polyimide-based material as a binder.
  • the secondary battery includes a water-soluble polyamide-based material and a water-soluble thickener.
  • the surface tension of water can be lowered by adding a water-soluble thickener, and peeling of the negative electrode mixture layer can be suppressed.
  • the amount of the thickener soluble in water is 0.3 wt% or more with respect to the sum of the weights of the active material, the binder, and the thickener, and the amount of the binder is the active material, the It is 3 to 15 wt% with respect to the sum of the weights of the binder and the thickener.
  • the amount of the binder is A and the amount of the thickener is B, it is desirable to satisfy (Equation 1).
  • the type of the thickener includes at least one of cellulose, polyethylene glycol polyacrylamide, and poly N-vinylamide. More preferably, the binder is polyamideimide and the thickener is carboxymethylcellulose.
  • Polyimide-based materials and polyamide-based materials generally require a curing treatment of 200 ° C. or more, and thus require a large vacuum dryer to suppress oxidation of the current collector foil.
  • a desirable molecular structure of the binder includes two or more double bonds of oxygen. The oxygen double bond is water-soluble and therefore soluble in water.
  • the capacity of the lithium ion secondary battery is increased and the ease of electrode production is improved.
  • the physical property value of the negative electrode binder of an Example and a comparative example, and the physical property value of a negative electrode current collecting plate It is an exploded view of the laminated electrode group inside a laminate cell. It is a disassembled perspective view of a laminate cell. It is a figure which shows the discharge capacity measurement result of a negative electrode. The figure which shows the relationship between the amount of binders, the amount of thickeners, and the electrode state of a negative electrode. The figure which shows the capacity
  • the present invention will be described with reference to examples.
  • the present invention is not limited to the examples described below.
  • the lamination-type laminate cell is used this time, the same effect can be obtained regardless of whether it is an other winding structure or a metal can sealed.
  • Example (Negative electrode active material, negative electrode binder and thickener)
  • the negative electrode active material an active material in which an active material containing Si and graphite were mixed at a weight ratio of 1: 1 was used.
  • the active material containing Si materials such as Si alloy and Si oxide can be used. This time, Si alloy was used.
  • the Si alloy is usually in a state where fine particles of metal silicon (Si) are dispersed in each particle of other metal elements, or a state in which other metal elements are dispersed in each particle of Si. It has become.
  • Other metal elements may be used as long as they contain at least one of Al, Ni, Cu, Fe, Ti, and Mn.
  • the Si alloy can be produced by mechanically synthesizing by a mechanical alloy method, or by heating and cooling a mixture of Si particles and other metal elements. This time, the former one was used.
  • the composition of the Si alloy the atomic ratio of Si: other metal elements is desirably 50:50 to 90:10, and more desirably 60:40 to 80:20.
  • Si 70 Ti 30 was used as 70:30, but Si 70 Ti 10 Fe 10 Al 10 , Si 70 Al 30 , Si 70 Ni 30 , Si 70 Cu 30 , Si 70 Fe 30 , Si 70 Ti 30 , Si 70 Mn 30 , Si 70 Ti 15 Fe 15 , Si 70 Al 10 Ni 20 or the like may be used.
  • graphite materials such as natural graphite and artificial graphite can be used. Natural graphite is desirable from the viewpoint of cost, but the surface may be coated with non-graphitizable carbon. This time, natural graphite having d002 of 3.356 mm or less, Lc (002) of 1000 mm or more, and La (110) of 1000 mm or more was used as crystallinity.
  • the binder used here is water-soluble polyamideimide, but water-soluble polyamide, water-soluble polyimide, or a mixture thereof may be used.
  • the structural example of water-soluble polyamideimide is shown in Formula 1.
  • X and Y are organic groups. Since the oxygen double bond shown in the formula is an immersion group, it becomes soluble in water.
  • thickener carboxymethylcellulose, polyethylene glycol polyacrylamide, and poly N-vinylamide were used at this time, but an aqueous thickener or a mixture thereof may be used.
  • FIG. 1 shows active material types, solvents, thickener types, thickener amounts, and binder amounts of the examples and comparative examples used this time.
  • the negative electrode was prepared by preparing a negative electrode mixture slurry, coating the material on a current collector plate, and pressing.
  • the negative electrode slurry uses acetylene black (d) as a conductive material in addition to the negative electrode active material (a), binder (b) and thickener (c) described above, and the weight ratio of the negative electrode active material is 100-b-
  • a slurry was prepared while mixing the solvent such that c-dwt% and acetylene black were prepared at 3 wt% and the solid content ratio was 50 wt%.
  • a planetary mixer was used for slurry preparation.
  • coating was performed on the current collector plate foil with a desktop comma coater.
  • the coating amount was prepared to be 11 g / m2.
  • the drying temperature was dried through a 90 ° C. drying oven.
  • the separator is not particularly limited as long as it is a material that does not allow lithium ions to pass through due to thermal contraction.
  • polyolefin is used.
  • Polyolefin is mainly characterized by containing at least one kind of polyethylene, polypropylene, etc., but may contain heat-resistant resin such as polyamide, polyamideimide, polyimide, polysulfone, polyethersulfone, polyphenylsulfone, polyacrylonitrile. Absent.
  • an inorganic filler layer may be applied on one side or both sides.
  • the inorganic filler layer is characterized by containing at least one of SiO 2 , Al 2 O 3 , montmorillonite, mica, ZnO, TiO 2 , BaTiO 3 , and ZrO 2. From the viewpoint of cost and performance, SiO 2 or Al 2 O 3 is most preferred. This time, a three-layer film having a thickness of 25 ⁇ m having polyethylene between polypropylenes was used.
  • electrolytes include, for example, ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, ethyl methyl carbonate, diethyl carbonate, ⁇ -butyrolactone, ⁇ -valerolactone, methyl acetate, ethyl acetate, methyl propionate, tetrahydrofuran, 2 -Methyltetrahydrofuran, 1,2-dimethoxyethane, 1-ethoxy-2-methoxyethane, 3-methyltetrahydrofuran, 1,2-dioxane, 1,3-dioxane, 1,4-dioxane, 1,3-dioxolane, 2 -Non-aqueous solvent selected from at least one selected from methyl-1,3-dioxolane, 4-methyl-1,3-dioxolane, etc., for example, LiPF 6 , LiBF 4 , LiClO 4 , LiN (C 2 F
  • the positive electrode has an aluminum foil as a positive electrode current collector foil.
  • a positive electrode mixture layer is formed on the aluminum foil.
  • the positive electrode active material mixture includes LiNi 1/3 Mn 1/3 Co 1/3 O 2 as a positive electrode active material, a conductive material of carbon material, and A binder (binder) of polyvinylidene fluoride (hereinafter abbreviated as PVDF) was used.
  • the weight ratio was 90: 5: 5 in order, and the mixture coating amount was 240 g / m 2 .
  • the positive electrode active material mixture is applied to the aluminum foil, the viscosity is adjusted with a dispersion solvent of N-methyl-2-pyrrolidone.
  • the positive electrode after coating was dried at 120 ° C., and the density was adjusted by a roll press, and this time the density was 3.0 g / cm 3 .
  • FIG. 2 shows an exploded view of the laminated electrode group inside the laminated cell.
  • a stacked electrode group inside the laminate cell was first prepared.
  • a plate-like positive electrode 5 and a strip-like negative electrode 6 are sandwiched and stacked between separators 7.
  • the number of stacked layers was adjusted so that the thickness of the electrode group was 2 mm.
  • the produced positive electrode and negative electrode each formed an uncoated part where the active material mixture was not applied on a part of the foil during processing.
  • the positive electrode uncoated portion 3 and the negative electrode uncoated portion 4 are bundled and ultrasonically welded to the positive electrode terminal 1 and the negative electrode terminal 2 that electrically connect the inside and outside of the battery.
  • the welding method may be other welding methods such as resistance welding.
  • the positive terminal 1 and the negative terminal 2 may be preliminarily coated with or attached to a sealing portion of the terminal in order to further seal the inside and outside of the battery.
  • FIG. 3 shows an exploded perspective view of the laminate cell.
  • the positive electrode terminal 1 and the negative electrode terminal 2 are penetrated in a state where the electrode group 9 is heat-sealed and sealed for 10 seconds at 175 ° C. with the ridges of the laminate films 8 and 10 being electrically insulated.
  • the sealing was performed by heat welding and sealing while heat-welding first except one side and injecting the electrolytic solution, and then vacuum-pressing the remaining one side.
  • FIG. 4 shows the measurement results of the discharge capacity of the negative electrode.
  • Examples 1 to 6 and Comparative Examples 3 and 4 could be applied without any problem in the electrode state.
  • Comparative Examples 1 and 2 it could not be applied.
  • the active material layer includes a water-soluble polyimide-based material or a water-soluble polyamide-based material as a binder, By having a thickener soluble in water, the surface tension of water is lowered, and peeling of the negative electrode mixture layer can be suppressed.
  • the amount of the thickener soluble in water is 0.3 wt% or more based on the sum of the weights of the active material, the binder and the thickener from Example 1 and Comparative Example 1, and the amount of the binder is According to Examples 1 to 6, the content is 3 to 15 wt% with respect to the sum of the weights of the active material, the binder, and the thickener.
  • FIG. 5 shows the relationship among the binder amount, the thickener amount, and the electrode state of the negative electrode.
  • FIG. 6 shows the results of cell capacity measurement.
  • Examples 1 to 6 and Comparative Example 4 showed a capacity of 800 mAh, but Comparative Example 3 was found to be as low as 600 mAh. Since the comparative example 3 did not contain Si type material in an active material, it resulted in a low capacity
  • the active material layer in a secondary battery having a negative electrode mainly composed of an Si-based active material as an active material, can be used as a binder for water-soluble polyimide-based material or water-soluble polyamide-based material and water.
  • the amount of the thickener soluble in water is 0.3 wt% or more with respect to the sum of the weights of the active material, the binder and the thickener, 3 to 15 wt% with respect to the sum of weight.
  • Equation 1 is satisfied, which is the most desirable form.
  • the secondary battery described in the present invention has a negative electrode mainly composed of an Si-based active material as an active material, and the active material layer has a water-soluble polyimide-based material or a water-soluble polyamide-based material as a binder, and water. And a soluble thickener.
  • a thickener that is soluble in water, the binder does not aggregate and the mixture layer can be uniformly applied on the electrode.
  • the secondary battery according to the present invention is characterized in that the amount of the water-soluble thickener is 0.3 wt% or more with respect to the sum of the weights of the active material, the binder and the thickener. .
  • the amount of the binder is 3 to 15 wt% with respect to the sum of the weights of the active material, the binder and the thickener.
  • the secondary battery according to the present invention is characterized by satisfying (Equation 1) when the amount of the binder is A and the amount of the thickener is B.
  • Equation 1 A-5.3B -0.85 ⁇ 0 (Equation 1)
  • the thickener includes at least one of cellulose, polyethylene glycol polyacrylamide, and poly N-vinylamide.
  • the binder is polyamideimide
  • the thickener is carboxymethylcellulose
  • the binder contains two or more double bonds of oxygen.
  • the secondary battery according to the present invention has a negative electrode mainly composed of an Si-based active material as an active material, and the active material layer has a water-soluble polyimide-based material or a water-soluble polyamide-based material as a binder, A thickener that is soluble in water.
  • the present invention is not limited to the above-described embodiments, and various designs can be made without departing from the spirit of the present invention described in the claims. It can be changed.
  • the above-described embodiment has been described in detail for easy understanding of the present invention, and is not necessarily limited to one having all the configurations described.
  • a part of the configuration of an embodiment can be replaced with the configuration of another embodiment, and the configuration of another embodiment can be added to the configuration of an embodiment.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Materials Engineering (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

Selon l'invention, des tentatives d'amélioration de la durée de vie à l'aide de polyamides, de polyimides et de polyamide-imides en tant que liants et par suppression de l'expansion et de la contraction ont été menées, mais puisque dans les liants susmentionnés le solvant utilisé est un solvant organique tel que la NMP et en raison de préoccupations environnementales, un équipement tel qu'un conduit d'évacuation fut requis, entraînant une augmentation des coûts. Par ailleurs, des polyamides solubles dans l'eau dissous dans de l'eau ou similaire ont récemment été étudiés, permettant l'anticipation d'une réduction des coûts. Cependant, étant donné que le solvant utilisé dans les polyamides solubles dans l'eau est l'eau, la tension superficielle est élevée par rapport aux solvants organiques (par exemple, la NMP), le liant s'agglutine pendant la production d'électrode, et la couche de mélange d'électrode négative se détache. La pile rechargeable de la présente invention comprend une électrode négative dans laquelle un matériau actif à base de Si est utilisé en tant que matériau primaire du matériau actif, la pile rechargeable étant caractérisée en ce que la couche de matériau actif comprend un matériau polyimide ou polyamide soluble dans l'eau en tant que liant, et un épaississant soluble dans l'eau.
PCT/JP2017/027607 2016-09-30 2017-07-31 Pile rechargeable au lithium-ion Ceased WO2018061457A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2016195187A JP6718784B2 (ja) 2016-09-30 2016-09-30 リチウムイオン二次電池
JP2016-195187 2016-09-30

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Publication number Priority date Publication date Assignee Title
US11018342B2 (en) 2017-03-15 2021-05-25 Nec Corporation Binder composition for secondary battery
JP7707531B2 (ja) * 2020-01-28 2025-07-15 株式会社リコー 電気化学素子作製用非水系液体組成物、電極の製造方法、電気化学素子の製造方法及び電極
JP2021136226A (ja) * 2020-02-28 2021-09-13 Tdk株式会社 負極活物質層形成用組成物、およびそれを用いた負極およびリチウムイオン二次電池

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007095670A (ja) * 2005-08-29 2007-04-12 Matsushita Electric Ind Co Ltd 非水電解質二次電池用負極およびその製造方法、ならびに非水電解質二次電池
JP2012109143A (ja) * 2010-11-18 2012-06-07 Du Pont Mitsui Fluorochem Co Ltd 電池正極及びリチウムイオン二次電池
JP2013256666A (ja) * 2013-07-26 2013-12-26 Toray Ind Inc ポリイミド系樹脂水溶液
JP2014044895A (ja) * 2012-08-28 2014-03-13 Honda Motor Co Ltd 電解質−負極構造体及びそれを備えるリチウムイオン二次電池
JP2015204133A (ja) * 2014-04-10 2015-11-16 株式会社カネカ 水系バインダ組成物

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007095670A (ja) * 2005-08-29 2007-04-12 Matsushita Electric Ind Co Ltd 非水電解質二次電池用負極およびその製造方法、ならびに非水電解質二次電池
JP2012109143A (ja) * 2010-11-18 2012-06-07 Du Pont Mitsui Fluorochem Co Ltd 電池正極及びリチウムイオン二次電池
JP2014044895A (ja) * 2012-08-28 2014-03-13 Honda Motor Co Ltd 電解質−負極構造体及びそれを備えるリチウムイオン二次電池
JP2013256666A (ja) * 2013-07-26 2013-12-26 Toray Ind Inc ポリイミド系樹脂水溶液
JP2015204133A (ja) * 2014-04-10 2015-11-16 株式会社カネカ 水系バインダ組成物

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