Method of manufacturing high-ion conductive sulfide-based solid electrolyte using dissolution-precipitation and composition used therefor

Patent metadata

Field	Value
Publication number	US-10991977-B2
Application number	US-201916661796-A
Country	US
Kind code	B2
Filing date	Oct 23, 2019
Priority date	Nov 30, 2018
Publication date	Apr 27, 2021
Grant date	Apr 27, 2021

Abstract

A method of manufacturing a high-ion conductive sulfide-based solid electrolyte using dissolution-precipitation includes preparing a composite solvent including a first solvent including a cyano group and a second solvent having a polarity index of less than 4, introducing a raw material including lithium sulfide (Li2S) and phosphorus pentasulfide (P2S5) into the composite solvent, and stirring the raw material to obtain a sulfide precipitate.

First claim

What is claimed is:

1. A composition for preparing a sulfide-based solid electrolyte, the composition comprising:
a composite solvent comprising a first solvent comprising a cyano group and a second solvent having a polarity index of less than 4; and
a raw material comprising lithium sulfide (Li 2 S) and phosphorus pentasulfide (P 2 S 5 ),
wherein the composite solvent comprises 99.975 wt % or more to less than 100 wt % of the first solvent and more than 0 wt % to 0.025 wt % or less of the second solvent.

2. The composition of claim 1 , wherein the first solvent is acetonitrile.

3. The composition of claim 1 , wherein the second solvent is selected from a group consisting of isopropyl alcohol, 2-butanol, and a combination thereof.

4. The composition of claim 1 , wherein the raw material further comprises lithium halide (LiX, wherein X is a halogen element).

5. The composition of claim 4 , wherein the raw material comprises 50 mol % to 62.5 mol % of lithium sulfide (Li 2 S), 12.5 mol % to 20 mol % of phosphorus pentasulfide (P 2 S 5 ), and 25 mol % to 37.5 mol % of lithium halide (LiX).

6. A method of manufacturing a sulfide-based solid electrolyte, the method comprising:
preparing a composite solvent comprising a first solvent comprising a cyano group and a second solvent having a polarity index of less than 4;
introducing a raw material comprising lithium sulfide (Li 2 S) and phosphorus pentasulfide (P 2 S 5 ) into the composite solvent to form a mixture; and
stirring the mixture to obtain a sulfide precipitate,
wherein the composite solvent comprises 99.975 wt % or more to less than 100 wt % of the first solvent and more than 0 wt % to 0.025 wt % or less of the second solvent.

7. The method of claim 6 , further comprising removing the composite solvent.

8. The method of claim 7 , further comprising thermally treating the sulfide precipitate to crystallize the sulfide precipitate after removing the composite solvent.

9. The method of claim 6 , wherein the first solvent is acetonitrile.

10. The method of claim 6 , wherein the second solvent is selected from a group consisting of isopropyl alcohol, 2-butanol, and a combination thereof.

11. The method of claim 6 , wherein the raw material further comprises lithium halide (LiX, wherein X is a halogen element).

12. The method of claim 11 , wherein the raw material comprises 50 mol % to 62.5 mol % of lithium sulfide (Li 2 S), 12.5 mol % to 20 mol % of phosphorus pentasulfide (P 2 S 5 ), and 25 mol % to 37.5 mol % of lithium halide (LiX).

13. The method of claim 6 , wherein the stirring is performed at a temperature of 30 to 80° C.

14. The method of claim 6 , wherein the stirring comprises first stirring performed under conditions of 100 to 150 rpm and 5 to 10 minutes and second stirring performed under conditions of 250 to 300 rpm and 18 to 48 hours.

15. The method of claim 14 , wherein the first stirring and the second stirring are continuously performed.

16. The method of claim 6 , wherein the composite solvent is removed through vacuum drying under conditions of 30 to 80° C. and 1 to 24 hours.

17. The method of claim 6 , wherein the sulfide precipitate is crystallized through heat treatment performed under conditions of 300 to 550° C. and 1 to 48 hours.

18. The method of claim 8 , wherein the sulfide-based solid electrolyte has an argyrodite-type crystalline structure.

Assignees

• Hyundai Motor Co Ltd
• Kia Motors Corp
• Univ Hanyang Ind Univ Coop Found

Inventors

• Seong Ju Yeong
• Song In Woo
• Min Hong Seok
• Jang Yong Jun
• Kim Yun Sung
• Shin Dong Wook
• Choi Sun Ho
• Ann Ji U
• Do Ji Yae
• Lim Seung Woo

Classifications

• C01B25/14 Primary

  Sulfur, selenium, or tellurium compounds of phosphorus · CPC title

• H01M2300/0068

  inorganic · CPC title

• H01M10/0562 Primary

  Solid materials · CPC title

• Y02E60/10

  Energy storage using batteries · CPC title

• H01M10/052

  Li-accumulators · CPC title