Solid electrolyte and preparing method thereof

Patent metadata

Field	Value
Publication number	US-10868330-B2
Application number	US-201715813673-A
Country	US
Kind code	B2
Filing date	Nov 15, 2017
Priority date	Nov 16, 2016
Publication date	Dec 15, 2020
Grant date	Dec 15, 2020

Abstract

A method of preparing a solid electrolyte includes preparing a mixed powder with a sulfur powder, a phosphorus powder and a lithium powder. The sulfur in the sulfur powder, the phosphorus in the phosphorus powder, and the lithium in the lithium powder are each in an elemental form. The mixed powder is milled to obtain an amorphous powder. The method includes heat-treating the amorphous powder to form a crystallized solid electrolyte.

First claim

What is claimed is:

1. A method of preparing a solid electrolyte, the method comprising:
preparing a mixed powder comprising a sulfur powder, a phosphorus powder, a lithium powder, and a nickel powder, wherein the sulfur in the sulfur powder, the phosphorus in the phosphorus powder, the lithium in the lithium powder, and the nickel in the nickel powder are each in an elemental form;
milling the mixed powder to obtain an amorphous powder; and
heat-treating the amorphous powder to form a crystallized solid electrolyte, wherein the sulfur powder, the phosphorus powder, the lithium powder, and the nickel powder are mixed according to a composition of Li a P b S c Ni d (12≤a≤18, 0.8≤b≤6.4, 13.2≤c≤26, 1.2≤d≤9.6).

2. The method of claim 1 , wherein the mixed powder consists of the sulfur powder, the phosphorus powder, and the lithium powder.

3. The method of claim 1 , wherein the amorphous powder is obtained by milling the mixed powder under conditions of 300 RPM to 1000 RPM and 4 hrs to 40 hrs by using a planetary mill.

4. A method of preparing a solid electrolyte, the method comprising:
preparing a mixed powder comprising a sulfur powder, a phosphorus powder, a lithium powder, and a nickel powder, wherein the sulfur in the sulfur powder, the phosphorus in the phosphorus powder, the lithium in the lithium powder, and the nickel in the nickel powder are each in an elemental form;
milling the mixed powder to obtain an amorphous powder, wherein the milling comprises:
forming a slurry by mixing a 1 wt % to 50 wt % of the mixed powder with 50 wt % to 99 wt % of a solvent and then wet milling the slurry to obtain the amorphous powder; and
heat-treating the amorphous powder to form a crystallized solid electrolyte, wherein heat-treating the amorphous powder comprises heat-treating the wet milled slurry, wherein the sulfur powder, the phosphorus powder, the lithium powder, and the nickel powder are mixed according to a composition of Li a P b S c Ni d (12≤a≤18, 0.8≤b≤6.4, 13.2≤c≤26, 1.2≤d=9.6).

5. The method of claim 4 , wherein the solvent is at least one selected from a group consisting of:
at least one hydrocarbon-based solvent of pentane, hexane, 2-ethyl hexane, heptane, octane, cyclohexane, and methyl cyclohexane;
at least one BTX-based solvent of benzene, toluene, xylene, and ethylbenzene;
at least one ether-based solvent of diethyl ether, tetrahydrofuran, and 1,4-dioxane;
at least one ester-based solvent of ethyl propionate, and propyl propionate; or a mixture thereof.

6. The method of claim 1 , wherein the milling comprises dry milling.

7. The method of claim 1 , wherein the heat-treating comprises heat-treating the amorphous powder at 200° C. to 500° C. and 1 min to 100 hrs.

8. The method of claim 1 , wherein the preparing, the milling, and the heat-treating are performed in a dry room.

9. A method of preparing a solid electrolyte, the method comprising:
preparing a mixed powder comprising a sulfur powder, a phosphorus powder, a lithium powder, and a nickel powder, wherein the sulfur in the sulfur powder, the phosphorus in the phosphorus powder, the lithium in the lithium powder, and the nickel in the nickel powder are each in an elemental form;
adding the mixed powder in to a solvent;
wet milling the mixed powder in the solvent, wherein the wet milling amorphizes the mixed powder in the solvent; and
heat-treating the amorphized mixed powder in the solvent, wherein the heat-treating removes the solvent and crystallizes the amorphized mixed powder to form the solid electrolyte,
wherein the sulfur powder, the phosphorus powder, the lithium powder, and the nickel powder are mixed according to a composition of LiaPbScNid (12≤a≤18, 0.8≤b≤6.4, 13.2≤c≤26, 1.2≤d≤9.6).

10. The method of claim 9 , wherein the mixed powder consists of the sulfur powder, the phosphorus powder, and the lithium powder.

11. The method of claim 9 , wherein the wet milling comprises milling the mixed powder under conditions of 300 RPM to 1000 RPM and 4 hrs to 40 hrs by using a planetary mill.

12. The method of claim 9 , wherein adding the mixed powder in to the solvent comprises:
mixing a 1 wt % to 50 wt % of the mixed powder with 50 wt % to 99 wt % of the solvent.

13. The method of claim 9 , wherein the solvent is a solvent selected from a group consisting of:
a hydrocarbon-based solvent of pentane, hexane, 2-ethyl hexane, heptane, octane, cyclohexane, or methyl cyclohexane;
a BTX-based solvent of benzene, toluene, xylene, or ethylbenzene;
an ether-based solvent of diethyl ether, tetrahydrofuran, or 1,4-dioxane; and
an ester-based solvent of ethyl propionate, or propyl propionate.

14. The method of claim 9 , wherein the heat-treating comprises heat-treating at 200° C. to 500° C. and 1 min to 100 hrs.

15. The method of claim 9 , wherein the preparing, the adding, the wet milling, and the heat-treating are performed in a dry room.

16. The method of claim 4 , wherein the mixed powder consists of the sulfur powder, the phosphorus powder, and the lithium powder.

17. The method of claim 4 , wherein the amorphous powder is obtained by milling the mixed powder under conditions of 300 RPM to 1000 RPM and 4 hrs to 40 hrs by using a planetary mill.

18. The method of claim 4 , wherein the heat-treating comprises heat-treating the amorphous powder at 200° C. to 500° C. and 1 min to 100 hrs.

19. The method of claim 4 , wherein the preparing, the milling, and the heat-treating are performed in a dry room.

Assignees

• Hyundai Motor Co Ltd
• Kia Motors Corp

Inventors

• Sung Ju Young
• Lim Jae Min
• Jang Yong Jun

Classifications

• C01G53/82

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

• Y02E60/10

  Energy storage using batteries · CPC title

• C01B17/22

  Alkali metal sulfides or polysulfides · CPC title

• H01M2300/0068

  inorganic · CPC title

• H01M10/052

  Li-accumulators · CPC title