# US 11,444,316 B2 · Solid electrolyte and all-solid battery

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- Number: US 11,444,316 B2
- Document ID: US11444316B2
- Status: Granted
- Kind: B2
- Application number: 16/007,008
- Filed: 2018-06-13
- Published: 2018-10-11
- Granted: 2022-09-13
- Earliest claimed: 2016-02-05
- Assignees: Murata Manufacturing Co., Ltd.
- Applicants: Murata Manufacturing Co., Ltd.
- Inventors: Ryohei Takano; Makoto Yoshioka; Takeo Ishikura; Akisuke Ito
- Web page: https://patentgrep.com/patent/US11444316B2

## CPC

- H01M 10/0562: Solid materials
- C04B 35/01: based on oxide ceramics
- C04B 35/62615: {High energy or reactive ball milling}
- C04B 35/62635: {Mixing details}
- C04B 35/6264: {Mixing media, e.g. organic solvents}
- C04B 35/62645: {Thermal treatment of powders or mixtures thereof other than sintering}
- C04B 35/62685: {characterised by the order of addition of constituents or additives}
- C04B 35/63408: {Polyalkenes}
- H01M 4/0471: {involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis}
- H01M 10/052: Li-accumulators
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 10/0585: of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
- C04B 2235/3203: Lithium oxide or oxide-forming salts thereof
- C04B 2235/3206: Magnesium oxides or oxide-forming salts thereof
- C04B 2235/3217: Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
- C04B 2235/3224: Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
- C04B 2235/3227: Lanthanum oxide or oxide-forming salts thereof
- C04B 2235/3244: Zirconium oxides, zirconates, hafnium oxides, hafnates, or oxide-forming salts thereof
- C04B 2235/3284: Zinc oxides, zincates, cadmium oxides, cadmiates, mercury oxides, mercurates or oxide forming salts thereof
- C04B 2235/3286: Gallium oxides, gallates, indium oxides, indates, thallium oxides, thallates or oxide forming salts thereof, e.g. zinc gallate
- C04B 2235/604: Pressing at temperatures other than sintering temperatures
- C04B 2235/764: Garnet structure A3B2(CO4)3
- C04B 2235/77: Density
- H01M 2300/0071: Oxides
- H01M 2300/0077: based on zirconium oxide
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- C04B: LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE {(roofing granules E04D7/005)}; CERAMICS (devitrified glass-ceramics C03C10/00); REFRACTORIES; TREATMENT OF NATURAL STONE
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A solid electrolyte having a garnet type crystal structure. The garnet type crystal structure contains Li, La, Zr, O and Ga and at least one element selected from Al, Mg, Zn and Sc.

## Claims

### Claim 1

A solid electrolyte comprising a garnet type crystal structure represented by (Li7−(3x+3y)GaxScy)La3Zr2O12 where α is a valence of Sc, and 0<x<0.3, 0<y<0.3, 0.4<3x+ay<0.9.

### Claim 2 (depends on 1)

The solid electrolyte according to claim 1, wherein
a first content of Ga is more than 0 mol % and less than 13.4 mol % with respect to a second content of La,
a total of a third content of the Sc is more than 0 mol % and less than 13.4 mol % with respect to the second content of La, and
a total of the first content of Ga and the third content of the Sc is more than 0.30 mol % and less than 20 mol % in the garnet type crystal structure.

### Claim 3 (depends on 2)

The solid electrolyte according to claim 2, wherein
the first content of Ga is more than 0.66 mol % and less than 6.67 mol % with respect to the second content of La,
the total of the third content of the Sc is more than 0 mol % and less than 6.67 mol % with respect to the second content of La, and
the total of the first content of Ga and the third content of the Sc is more than 0.33 mol % and less than 10 mol % in the garnet type crystal structure.

### Claim 4 (depends on 3)

The solid electrolyte according to claim 3, wherein
a fourth content of Zr is 50 mol % to 80 mol % with respect to the second content of La, and
a fifth content of Li is 197 mol % to 280 mol % with respect to the second content of La.

### Claim 5 (depends on 4)

The solid electrolyte according to claim 4, wherein
the fourth content of Zr is 60 mol % to 70 mol % with respect to the second content of La, and
the fifth content of Li is 203 mol % to 220 mol % with respect to the second content of La.

### Claim 6 (depends on 1)

The solid electrolyte according to claim 1, wherein a first content of Ga is more than 0 mol % and less than 13.4 mol % with respect to a second content of La.

### Claim 7 (depends on 6)

The solid electrolyte according to claim 6, wherein the first content of Ga is more than 0.66 mol % and less than 6.67 mol % with respect to the second content of La.

### Claim 8 (depends on 1)

The solid electrolyte according to claim 1, wherein a total of a first content of the Sc is more than 0 mol % and less than 13.4 mol % with respect to a second content of La.

### Claim 9 (depends on 8)

The solid electrolyte according to claim 8, wherein the total of the first content of the Sc is more than 0 mol % and less than 6.67 mol % with respect to the second content of La.

### Claim 10 (depends on 1)

The solid electrolyte according to claim 1, wherein a total of a first content of Ga and a second content of the Sc is more than 0.30 mol % and less than 20 mol % in the garnet type crystal structure.

### Claim 11 (depends on 10)

The solid electrolyte according to claim 10, wherein the total of the first content of Ga and the second content of the Sc is more than 0.33 mol % and less than 10 mol % in the garnet type crystal structure.

### Claim 12 (depends on 1)

The solid electrolyte according to claim 1, wherein a first content of Zr is 50 mol % to 80 mol % with respect to a second content of La.

### Claim 13 (depends on 12)

The solid electrolyte according to claim 12, wherein the first content of Zr is 60 mol % to 70 mol % with respect to the second content of La.

### Claim 14 (depends on 1)

The solid electrolyte according to claim 1, wherein a first content of Li is 197 mol % to 280 mol % with respect to a second content of La.

### Claim 15 (depends on 14)

The solid electrolyte according to claim 14, wherein the first content of Li is 203 mol % to 220 mol % with respect to the second content of La.

### Claim 16 (depends on 1)

An all-solid battery comprising:
a solid electrolyte layer containing the solid electrolyte according to claim 1;
a positive electrode joined to a first surface of the solid electrolyte layer; and
a negative electrode joined to a second surface of the solid electrolyte layer.

### Claim 17 (depends on 16)

The all-solid battery according to claim 16, wherein
a first content of Ga is more than 0 mol % and less than 13.4 mol % with respect to a second content of La,
a total of a third content of the Sc is more than 0 mol % and less than 13.4 mol % with respect to the second content of La, and
a total of the first content of Ga and the third content of the Sc is more than 0.30 mol % and less than 20 mol % in the garnet type crystal structure.

### Claim 18 (depends on 17)

The all-solid battery according to claim 17, wherein
the first content of Ga is more than 0.66 mol % and less than 6.67 mol % with respect to the second content of La,
the total of the third content of the Sc is more than 0 mol % and less than 6.67 mol % with respect to the second content of La, and
the total of the first content of Ga and the third content of the Sc is more than 0.33 mol % and less than 10 mol % in the garnet type crystal structure.