Method of preparing sulfide-based solid electrolyte for all-solid battery having argyrodite-type crystal structure

Patent metadata

Field	Value
Publication number	US-10903518-B2
Application number	US-201816160150-A
Country	US
Kind code	B2
Filing date	Oct 15, 2018
Priority date	Dec 6, 2017
Publication date	Jan 26, 2021
Grant date	Jan 26, 2021

Abstract

Disclosed is a method of preparing a sulfide-based solid electrolyte for an all-solid battery having an argyrodite-type crystal structure through a solution process. The method including obtaining a precursor solution by dissolving lithium sulfide, phosphorus sulfide and a halogen compound in a solvent, obtaining a precursor powder by removing the solvent from the precursor solution. Solid electrolyte for an all-solid battery can be produced by such method.

First claim

What is claimed:

1. A method of preparing a sulfide-based solid electrolyte for an all-solid battery, comprising:
obtaining a precursor solution by admixing lithium sulfide, phosphorus sulfide and a halogen compound in a solvent;
obtaining a precursor powder by removing at least a portion of the solvent from the precursor solution; and
thermally treating the precursor powder,
wherein the solvent is removed by subjecting the precursor solution in a vacuum atmosphere to first drying at a temperature ranging from about 25° C. to less than about 50° C. for about 1 hr to 3 hr, second drying at a temperature ranging from about 50° C. to less than about 100° C. for about 1 hr to 3 hr, third drying at a temperature ranging from about 100° C. to less than about 150° C. for about 1 hr to 3 hr, fourth drying at a temperature ranging from about 150° C. to less than about 200° C. for about 1 hr to 3 hr, and/or fifth drying at a temperature ranging from about 200° C. to less than about 250° C. for about 1 hr to 3 hr, two or more of the first drying to the fifth drying are performed under continuous or non-continuous heating.

2. The method of claim 1 , wherein solid electrolyte crystals are grown during or after thermally treating the precursor powder.

3. The method of claim 2 , wherein the grown solid electrolyte crystals comprise an argyrodite-type crystal structure.

4. The method of claim 1 , wherein the lithium sulfide comprises lithium sulfide (Li 2 S), and the phosphorus sulfide comprises phosphorus pentasulfide (P 2 S 5 ).

5. The method of claim 1 , wherein the halogen compound is selected from the group consisting of lithium bromide (LiBr), lithium chloride (LiCl), lithium iodide (LiI) and combinations thereof.

6. The method of claim 1 , wherein the solvent is selected from the group consisting of ethanol, propanol, butanol, dimethyl carbonate, ethyl acetate, tetrahydrofuran, 1,2-dimethoxyethane, propylene glycol dimethyl ether, acetonitrile and combinations thereof.

7. The method of claim 1 , wherein the solvent is removed by drying after obtaining the precursor solution.

8. The method of claim 1 , wherein the solvent is removed by drying the precursor solution in a vacuum atmosphere at a temperature ranging from about 25° C. to about 250° C. for about 5 hr to about 15 hr.

9. The method of claim 1 , wherein the precursor powder is thermally treated at a temperature of about 400° C. to 600° C. for about 1 hr to 5 hr.

10. The method of claim 9 , wherein the precursor powder is thermally treated by elevating a temperature from room temperature to about 150° C. at a rate of about 2.5° C./min-10° C./min, from about 150° C. to about 250° C. at a rate of about 2.5° C./min-5° C./min, from about 250° C. to about 400° C. at a rate of about 1° C./min-2.5° C./min, and/or from about 400° C. to about 550° C. at a rate of about 1° C./min.

11. The method of claim 1 , wherein the sulfide-based solid electrolyte comprises the argyrodite-type crystal structure, as represented by Chemical Formula 1:
[Chemical Formula 1]
Li 6 PS 5 X, wherein X is Cl, Br or I.

Assignees

• Hyundai Motor Co Ltd
• Kia Motors Corp

Inventors

• Jang Yong Jun
• Oh Pil Gun
• Min Hong Seok
• Yoon Yong Sub
• Kim Sa Heum
• Seong Ju Yeong

Classifications

• Y02E60/10

  Energy storage using batteries · CPC title

• H01M2300/0068

  inorganic · CPC title

• H01M10/0562 Primary

  Solid materials · CPC title

• H01M2300/008

  Halides · CPC title

• C01P2002/82

  by IR- or Raman-data · CPC title