Garnet powder, manufacturing method thereof, solid electrolyte sheet using hot press and manufacturing method thereof

Patent metadata

Field	Value
Publication number	US-2016049688-A1
Application number	US-201514716491-A
Country	US
Kind code	A1
Filing date	May 19, 2015
Priority date	Aug 18, 2014
Publication date	Feb 18, 2016
Grant date	—

Abstract

The present disclosure relates to garnet powder, a manufacturing method thereof, a solid electrolyte sheet using a hot press, and a manufacturing method thereof. In particular, the present disclosure provides a method for manufacturing Li 7 La 3 Zr 2 O 12 (LLZ) garnet powder including preparing a mixture by first dry mixing Li 2 CO 3 , La 2 O 3 , ZrO 2 , and Al 2 O 3 . The mixture is first calcinated for 5 to 7 hours in a temperature range of 800 to 1000° C. The calcinated mixture is ground to a powder with an average particle size of 1 to 4 μm through dry grinding. A cubic-phased LLZ garnet powder is prepared by second calcinating the ground mixture for 10 to 30 hours in a temperature range of 1100 to 1300° C.

First claim

What is claimed is:

1 . Li 7 La 3 Zr 2 O 12 (LLZ) garnet powder having a cubic-phased crystal structure, wherein a molar ratio of the Li:La:Zr atoms is 6.5 to 8.3:3:2.

2 . The LLZ garnet powder of claim 1 , wherein some of the Li is substituted with Al.

3 . The LLZ garnet powder of claim 2 , wherein the substituted Al is included in 0.02 to 1.075 mol, and the Al is doped in the form of Al 2 O 3 in 0.1 to 5% by weight with respect to the LLZ.

4 . A method for manufacturing Li 7 La 3 Zr 2 O 12 (LLZ) garnet powder comprising:
preparing a mixture by first dry mixing Li 2 CO 3 , La 2 O 3 , ZrO 2 , and Al 2 O 3 ; first calcinating the mixture for 5 to 7 hours in a temperature range of 800 to 1000° C.; grinding the calcinated mixture to a powder with an average particle size of 1 to 4 μm through dry grinding to form a ground mixture; and preparing a cubic-phased LLZ (Li 7 La 3 Zr 2 O 12 ) garnet powder by second calcinating the ground mixture for 10 to 30 hours in a temperature range of 1100 to 1300° C.

5 . The method for manufacturing LLZ garnet powder of claim 4 , wherein, in the LLZ garnet powder, a molar ratio of the Li 2 CO 3 , the La 2 O 3 , the ZrO 2 , and the Al 2 O 3 is 6.5 to 8.3:3:4:0.02 to 1.075.

6 . The method for manufacturing LLZ garnet powder of claim 4 , wherein, in the LLZ garnet powder, some of the Li is substituted with Al.

7 . The method for manufacturing LLZ garnet powder of claim 6 , wherein the substituted Al by doping Al 2 O 3 in 0.1 to 5% by weight with respect to the LLZ.

8 . The method for manufacturing LLZ garnet powder of claim 4 further comprising analyzing the LLZ garnet powder, wherein the analysis is carried out using X-Ray Diffraction (XRD), Raman Spectroscopy, or Inductively Coupled Plasma Mass Spectrometry (ICP-MS).

9 . A solid electrolyte sheet comprising the LLZ garnet powder of claim 1 .

10 . A solid electrolyte sheet comprising the LLZ garnet powder of claim 2 .

11 . A method for manufacturing a solid electrolyte sheet using a hot press, the method comprising:
preparing the LLZ garnet powder of claim 1 ; and manufacturing a solid electrolyte sheet by hot pressing the garnet powder for 30 minutes to 2 hours in a temperature range of 1050 to 1250° C. under an oxygen free atmosphere.

12 . The method for manufacturing a solid electrolyte sheet of claim 11 , wherein a thickness of the solid electrolyte sheet ranges from 0.01 to 5 mm.

13 . The method for manufacturing a solid electrolyte sheet of claim 11 , wherein ionic conductivity of the solid electrolyte sheet ranges from 6×10 −4 to 10×10 −4 S/cm.

14 . The method for manufacturing a solid electrolyte sheet of claim 11 , further comprising analyzing the solid electrolyte sheet, wherein the analysis is carried out using X-Ray Diffraction (XRD), Raman Spectroscopy, or Inductively Coupled Plasma Mass Spectrometry (ICP-MS).

15 . A method for manufacturing a solid electrolyte sheet using a hot press, the method comprising:
preparing the LLZ garnet powder of claim 2 ; and manufacturing a solid electrolyte sheet by hot pressing the garnet powder for 30 minutes to 2 hours in a temperature range of 1050 to 1250° C. under an oxygen free atmosphere.

16 . The method for manufacturing a solid electrolyte sheet of claim 15 , wherein a thickness of the solid electrolyte sheet ranges from 0.01 to 5 mm.

17 . The method for manufacturing a solid electrolyte sheet of claim 15 , wherein ionic conductivity of the solid electrolyte sheet ranges from 6×10 −4 to 10×10 −4 S/cm.

18 . The method for manufacturing a solid electrolyte sheet of claim 15 , further comprising analyzing the solid electrolyte sheet, wherein the analysis is carried out using X-Ray Diffraction (XRD), Raman Spectroscopy, or Inductively Coupled Plasma Mass Spectrometry (ICP-MS).

Assignees

• Hyundai Motor Co Ltd

Inventors

• Sung Ju Young
• Lee Ho Taek
• Kwon Eun Ji
• Jang Yong Jun
• Kim Ji Na

Classifications

• H01M10/0525

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

• C01B33/26

  Aluminium-containing silicates {, i.e. silico-aluminates} · CPC title

• H01M2300/0071

  Oxides · CPC title

• H01M10/0562 Primary

  Solid materials · CPC title

• C01G25/006

  Compounds containing zirconium, with or without oxygen or hydrogen, and containing two or more other elements · CPC title