# US 11,440,986 B2 · Solid electrolyte composition, binder for all-solid-state secondary batteries, and electrode sheet for batteries and all-solid-state secondary battery each using said solid electrolyte

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- Number: US 11,440,986 B2
- Document ID: US11440986B2
- Status: Granted
- Kind: B2
- Application number: 16/777,372
- Filed: 2020-01-30
- Published: 2020-06-11
- Granted: 2022-09-13
- Earliest claimed: 2013-09-25
- Assignees: FUJIFILM Corporation
- Applicants: FUJIFILM Corporation
- Inventors: Masaomi Makino; Hiroaki Mochizuki; Tomonori Mimura
- Web page: https://patentgrep.com/patent/US11440986B2

## CPC

- C08F 290/06: Polymers provided for in subclass C08G
- C08G 18/0823: {containing carboxylate salt groups or groups forming them}
- C08G 18/227: {of antimony, bismuth or arsenic}
- C08G 18/28: characterised by the compounds used containing active hydrogen
- C08G 18/282: {Alkanols, cycloalkanols or arylalkanols including terpenealcohols}
- C08G 18/2865: {Compounds having only one primary or secondary amino group; Ammonia}
- C08G 18/3206: {aliphatic}
- C08G 18/348: {Hydroxycarboxylic acids}
- C08G 18/44: Polycarbonates
- C08G 18/4833: {Polyethers containing oxyethylene units}
- C08G 18/5024: {containing primary and/or secondary amino groups}
- C08G 18/6692: {with compounds of group C08G18/34}
- C08G 69/26: derived from polyamines and polycarboxylic acids
- C08G 69/265: {from at least two different diamines or at least two different dicarboxylic acids}
- C08G 69/40: Polyamides containing oxygen in the form of ether groups (C08G69/12, C08G69/32 take precedence)
- C08G 69/42: Polyamides containing atoms other than carbon, hydrogen, oxygen, and nitrogen (C08G69/12, C08G69/32 take precedence)
- C08G 69/44: Polyester-amides
- C08G 73/10: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- C08G 73/1007: {from tetracarboxylic acids or derivatives and diamines}
- C08G 73/1042: {Copolyimides derived from at least two different tetracarboxylic compounds or two different diamino compounds}
- C08G 73/105: {with oxygen only in the diamino moiety}
- C08G 73/1082: {wholly aromatic in the tetracarboxylic moiety}
- C08L 33/26: Homopolymers or copolymers of acrylamide or methacrylamide
- H01M 4/13: Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M 4/62: Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M 4/622: {being polymers}
- H01M 10/0562: Solid materials
- H01B 1/06: mainly consisting of other non-metallic substances
- H01M 4/0404: {by coating on electrode collectors}
- H01M 6/18: with solid electrolyte
- H01M 2220/20: Batteries in motive systems, e.g. vehicle, ship, plane
- H01M 2300/0068: inorganic
- Y02E 60/10: Energy storage using batteries
- C08F: MACROMOLECULAR COMPOUNDS OBTAINED BY REACTIONS ONLY INVOLVING CARBON-TO-CARBON UNSATURATED BONDS
- C08G: MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08L: COMPOSITIONS OF MACROMOLECULAR COMPOUNDS (compositions based on polymerisable monomers C08F, C08G; artificial filaments or fibres D01F; textile treating compositions D06)
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01B: CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES (selection for magnetic properties H01F1/00; waveguides H01P {; printed circuits H05K})
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

Provided are a solid electrolyte composition including: an inorganic solid electrolyte having conductivity of an ion of metal belong to Group 1 or 2 in the periodic table; and a high polymer binder, in which the high polymer binder is formed of a polymer having a hard segment and a soft segment, a binder for all-solid-state secondary batteries, and an electrode sheet for batteries and an all-solid-state secondary battery each using the solid electrolyte composition.

## Claims

### Claim 1

A solid electrolyte composition comprising:
an inorganic solid electrolyte having conductivity of an ion of metal belong to Group 1 or 2 in the periodic table; and
a high polymer binder,
wherein the high polymer binder is formed of a polymer having a hard segment and a soft segment and further having, as a third component other than the hard segment and the soft segment, a repeating unit having a hetero atom-containing group having at least one functional group selected from the group consisting of a carboxylic acid group, a sulfonic acid group, a tertiary amino group, a cyano group, a hydroxyl group, and a metal alkoxide group, and
wherein a content of the repeating unit having the hetero atom-containing group is 5 mol % to 30 mol % in the total polymer.

### Claim 2 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein the hard segment forming the high polymer binder contains at least any one bond of an amide bond, an urea bond, an urethane bond, and an imide bond.

### Claim 3 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein the soft segment forming the high polymer binder contains at least any one of a polyalkylene oxide chain, a polycarbonate chain, a polyester chain, and a silicone chain.

### Claim 4 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein the polymer forming the high polymer binder includes a carbon-carbon unsaturated group.

### Claim 5 (depends on 4)

The solid electrolyte composition according to claim 4,
wherein the carbon-carbon unsaturated group is expressed by Formula (1) or (2) below,
in Formulae (1) and (2), each of R1 and R5 independently represents an oxygen atom or NRN, RN represents a hydrogen atom or an alkyl group, each of R2 to R4 and R6 to R10 independently represents a hydrogen atom or an alkyl group, and * represents a bonding position.

### Claim 6 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein the polymer forming the high polymer binder has at least any one of repeating structures expressed by Formulae (I-1) to (I-5) of Group I below, as the hard segment,
in Formulae (I-1) to (I-5), each of R11 and R12 independently represents a bivalent linking group which is an alkylene group, an arylene group, or a combination thereof, R13 represents an alkyl group, an alkenyl group, an aryl group, or an aralkyl group, R14 represents an aromatic or aliphatic tetravalent linking group, Ra represents a hydrogen atom or an alkyl group, and * represents a bonding position.

### Claim 7 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein the polymer forming the high polymer binder has at least any one of repeating structures expressed by Formulae (II-1) to (II-5) of Group II below, as the soft segment,
in Formulae (II-1) to (II-5), R21 represents a hydrogen atom or an alkyl group, R22 represents a substituent group which contains a polyalkylene oxide chain, a polycarbonate chain, or a polyester chain and of which a weight average molecular weight is 200 to 200,000, R23 represents a linking group which contains a polyalkylene oxide chain, a polycarbonate chain, or a polyester chain and of which a weight average molecular weight is 200 to 200,000, and * represents a bonding position.

### Claim 8 (depends on 1)

The solid electrolyte composition according to claim 1, further comprising:
an electrode active substance.

### Claim 9 (depends on 8)

The solid electrolyte composition comprising according to claim 8, wherein a ratio of a total mass of the inorganic solid electrolyte and the electrode active substance is in a range of 1,000 to 1 with respect to a mass of the high polymer binder.

### Claim 10 (depends on 1)

The solid electrolyte composition according to claim 1,
wherein a molar ratio of the soft segment component to the hard segment component forming the high polymer binder is 1 mol to 10,000 mol with respect to 100 mol of the hard segment component.

### Claim 11 (depends on 1)

An electrode sheet for batteries obtained by forming a film by disposing the solid electrolyte composition according to claim 1 on a metal foil.

### Claim 12 (depends on 1)

An all-solid-state secondary battery comprising:
a positive electrode active substance layer;
a negative active substance layer; and
a solid electrolyte layer,
wherein at least any one of the positive electrode active substance layer, the negative active substance layer, and the solid electrolyte layer is formed of the solid electrolyte composition according to claim 1.

### Claim 13 (depends on 1)

The solid electrolyte composition comprising according to claim 1, wherein a ratio of the inorganic solid electrolyte is in a range of 1,000 to 1 with respect to a mass of the high polymer binder.

### Claim 14

A solid electrolyte composition comprising:
an inorganic solid electrolyte having conductivity of an ion of metal belong to Group 1 or 2 in the periodic table; and
a high polymer binder,
wherein the high polymer binder is formed of a polymer having a hard segment and a soft segment and further having a third component other than the hard segment and the soft segment, and
wherein the polymer has a repeating structure expressed by Formula (3) below,
in Formula (3), R12a represents an arylene group having 6 to 22 carbon atoms, an alkylene group having 1 to 15 carbon atoms, and a combination thereof, R23a represents an alkylene group having 2 to 6 carbon atoms, R23b represents an alkylene group having an acidic group of which an acid dissociation constant pKa is 14 or less or a basic group in which a pKa of a conjugate acid is 14 or less, R23c represents an alkylene group having a radical or cationic polymerizable group, R23d represents a diol residue having a molecular weight of 500 to 10,000, and a glass-transition temperature of −100° C. to 50° C., x represents 40 mol % to 60 mol %, y1 represents 0 mol % to 40 mol %, y2 represents 1 mol % to 20 mol %, y3 represents 1 mol % to 40 mol %, y4 represents 1 mol % to 40 mol %, x+y1+y2+y3+y4 is 100 mol %, and * represents a bonding position.