Lithium composite oxide single crystal, lithium composite oxide polycrystal, lithium composite oxide material, solid electrolyte material, all- solid-state lithium-ion secondary battery, and method for producing solid electrolyte material

Patent metadata

Field	Value
Publication number	US-12467158-B2
Application number	US-202118252853-A
Country	US
Kind code	B2
Filing date	Nov 12, 2021
Priority date	Nov 17, 2020
Publication date	Nov 11, 2025
Grant date	Nov 11, 2025

Abstract

The lithium composite oxide single crystal has a chemical composition represented by Li 7-3x-w-v Ga x La 3 Zr 2-w-v Ta W Nb v O 12 (0.02≤x<0.5, 0≤W≤1.0, 0≤V≤1.0, and 0.05≤W+V≤1.0), which belongs to a space group I-43d in a cubic system and has a garnet structure.

First claim

What is claimed is:

1 . A lithium composite oxide single crystal having a chemical composition represented by Li 7-3x-w-v Ga x La 3 Zr 2-w-v Ta W Nb v O 12 (0.02≤x<0.5, 0≤W≤1.0, 0≤V≤1.0, and 0.05≤W+V≤1.0), which belongs to a space group I-43d in a cubic system and has a garnet structure.

2 . A lithium composite oxide polycrystal comprising:
a single crystal having a chemical composition represented by Li 7-3x-w-v Ga x La 3 Zr 2-w-v Ta W Nb v O 12 (0.02≤x<0.5, 0≤W≤1.0, 0≤V≤1.0, and 0.05≤W+V≤1.0), which belongs to a space group I-43d in a cubic system and has a garnet structure.

3 . The lithium composite oxide polycrystal according to claim 2 ,
wherein a relative density is 90% or more.

4 . The lithium composite oxide polycrystal according to claim 2 ,
wherein a relative density is 95% or more.

5 . A lithium composite oxide material comprising:
the lithium composite oxide single crystal according to claim 1 .

6 . A lithium composite oxide material comprising:
the lithium composite oxide polycrystal according to claim 2 .

7 . A solid electrolyte material comprising:
the lithium composite oxide single crystal according to claim 1 .

8 . A solid electrolyte material comprising:
the lithium composite oxide polycrystal according to claim 2 .

9 . The solid electrolyte material according to claim 8 ,
wherein a lithium ionic conductivity is 1.0×10 −3 S/cm or more.

10 . An all-solid-state lithium-ion secondary battery comprising:
a positive electrode; a negative electrode; and the solid electrolyte material according to claim 8 .

11 . A method for producing a solid electrolyte material, comprising:
a first step of melting a material having a chemical composition represented by Li (7-3x-W)y Ga xz La 3 Zr 2-W Ta W Nb v O 12 (0.02≤x<0.5, 1.1≤y≤1.4, 1.6≤z≤3.3, 0≤W≤1.0, 0≤V≤1.0, 0.05≤W+V≤1.0, 1.1≤y≤1.5, and 1.5≤z≤3.5), and producing the solid electrolyte material from the melted material.

12 . A method for producing a solid electrolyte material according to claim 11 , comprising:
a melted portion forming step, which is the first step, of melting at least a part of a rod-shaped base material containing a raw material having a chemical composition represented by Li (7-3x-W)y Ga xz La 3 Zr 2-W Ta W Nb v O 12 (0.02≤x<0.5, 1.1≤y≤1.4, 1.6≤z≤3.3, 0≤W≤1.0, 0≤V≤1.0, 0.05≤W+V≤1.0, 1.1≤y≤1.5, and 1.5≤z≤3.5) to form a melted portion; and a melted portion moving step of moving the melted portion at an average speed of 8 mm/h or more.

13 . The method for producing a solid electrolyte material according to claim 12 ,
wherein the average speed is 8 mm/h or more and 19 mm/h or less.

14 . The method for producing a solid electrolyte material according to claim 12 ,
wherein, in the melted portion forming step, the base material is rotated together with the melted portion at a rotation speed of 30 rpm or more in a plane perpendicular to a longitudinal direction.

15 . The method for producing a solid electrolyte material according to claim 12 ,
wherein the melted portion moving step is performed in a dry gas atmosphere in a state in which a seed crystal of a solid electrolyte is attached to the melted portion, and wherein the melted portion is solidified in the melted portion moving step, and wherein the dry gas atmosphere is oxygen, nitrogen, argon, or air.

16 . The method for producing a solid electrolyte material according to claim 12 ,
wherein, in the melted portion moving step, the melted portion is rotated at a rotation speed of 2 rpm or more and 8 rpm or less in a plane perpendicular to a longitudinal direction of the base material.

17 . A method for producing a solid electrolyte material according to claim 11 , comprising:
a melt forming step, which is the first step, of melting a raw material having a chemical composition represented by Li (7-3x-W)y Ga xz La 3 Zr 2-W Ta W Nb v O 12 (0.02≤x<0.5, 1.1≤y≤1.4, 1.6≤z≤3.3, 0≤W≤1.0, 0≤V≤1.0, 0.05≤W+V≤1.0, 1.1≤y≤1.5, and 1.5≤z≤3.5) in a crucible to form a melt of the raw material; a melt adhesion step of immersing a base material in the melt in the crucible and adhering the melt to the base material; and a melt moving step of moving the melt adhered to the base material together with the base material out of the crucible at an average speed of 8 mm/h or more.

18 . The method for producing a solid electrolyte material according to claim 17 ,
wherein the average speed is 8 mm/h or more and 19 mm/h or less.

19 . The method for producing a solid electrolyte material according to claim 17 ,
wherein the melt moving step is performed in a state in which a seed crystal of a solid electrolyte is attached to the base material.

20 . The method for producing a solid electrolyte material according to claim 17 ,
wherein, in the melt portion moving step, the base material having a rod shape is rotated at a rotation speed of 2 rpm or more and 8 rpm or less in a plane perpendicular to a longitudinal direction with respect to the melt.

Assignees

• Aist

Inventors

• Kataoka Kunimitsu
• Akimoto Junji

Classifications

• H01M2300/0071

  Oxides · CPC title

• H01M10/0562

  Solid materials · CPC title

• H01M10/0525

  Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries · CPC title

• C30B13/28

  Controlling or regulating · CPC title

• C30B13/14

  Crucibles or vessels · CPC title