Sulfide-based solid electrolyte and preparation method thereof

Patent metadata

Field	Value
Publication number	US-11063291-B2
Application number	US-201715482785-A
Country	US
Kind code	B2
Filing date	Apr 9, 2017
Priority date	Nov 22, 2016
Publication date	Jul 13, 2021
Grant date	Jul 13, 2021

Abstract

A sulfide-based solid electrolyte contains a nickel (Ni) element and a halogen element. For example, a sulfide-based solid electrolyte can include, with respect to 100 parts by mole of a mixture of lithium sulfide (Li2S) and diphosphorus pentasulfide (P2S5), 5 parts by mole to 20 parts by mole of nickel sulfide (Ni3S2), and 5 parts by mole to 40 parts by mole of lithium halide.

First claim

What is claimed is:

1. A method of preparing a sulfide-based solid electrolyte, the method comprising:
preparing a starting material by adding 5 parts by mole to 20 parts by mole of nickel sulfide (Ni 3 S 2 ) and 5 parts by mole to 40 parts by mole of lithium halide with respect to 100 parts by mole of a mixture of lithium sulfide (Li 2 S) and diphosphorus pentasulfide (P 2 S 5 );
milling the starting material to obtain an amorphous material; and
heat-treating the amorphous material at a temperature range of 200° C. to 260° C. or 400° C. to 600° C., wherein a crystallized sulfide-based solid electrolyte is obtained after the heat-treating, wherein the heat-treated sulfide-based solid electrolyte has a cubic crystal structure that has diffraction peaks in an area of diffraction angles 2θ of 15.5±0.5°, 18±0.5°, 25.5±0.5°, 30±0.5°, 31.5±0.5°, 40±0.5°, 45.5±0.5°, 48±0.5°, 53±0.5°, 55±0.5°, 56.5±0.5° and 59.5±0.5° in an X-ray diffraction spectrum.

2. The method of claim 1 , wherein the mixture comprises
60 mole % to 90 mole % of the lithium sulfide; and
10 mole % to 40 mole % of diphosphorus pentasulfide.

3. The method of claim 1 , wherein the lithium halide is expressed by LiX, where X is Cl, Br or I.

4. The method of claim 1 , wherein the heat-treating is performed at 400° C. to 600° C.

5. The method of claim 1 , wherein, the heat-treating is performed at 200° C. to 260° C.

6. The method of claim 3 , wherein X is Cl.

7. The method of claim 3 , wherein X is Br.

8. The method of claim 3 , wherein X is I.

9. The method of claim 1 , wherein the method forms a sulfide-based solid electrolyte having a cubic crystal structure and comprising:
with respect to 100 parts by mole of a mixture of lithium sulfide (Li 2 S) and diphosphorus pentasulfide (P 2 S 5 );
5 parts by mole to 20 parts by mole of nickel sulfide (Ni 3 S 2 ); and
5 parts by mole to 40 parts by mole of lithium halide.

10. The method of claim 9 , wherein the mixture comprises
60 mole % to 90 mole % of the lithium sulfide; and
10 mole % to 40 mole % of diphosphorus pentasulfide.

11. The method of claim 9 , wherein the lithium halide is expressed by LiX, where X is Cl, Br or I.

12. The method of claim 9 , wherein a crystallization temperature of the sulfide-based solid electrolyte is 200° C. to 260° C.

13. The method of claim 9 , wherein a crystallization temperature of the sulfide-based solid electrolyte is 400° C. to 600° C.

14. The method of claim 9 , wherein the sulfide-based solid electrolyte has high ion conductivity in a wide crystallization temperature range.

Assignees

• Hyundai Motor Co Ltd

Inventors

• Sung Ju Young
• Lee Ho Taek
• Lim Jae Min
• Jang Yong Jun

Classifications

• H01M10/0525 Primary

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

• H01M2300/0068

  inorganic · CPC title

• C01P2002/72

  by d-values or two theta-values, e.g. as X-ray diagram · CPC title

• C04B35/6264

  Mixing media, e.g. organic solvents · CPC title

• H01M10/052

  Li-accumulators · CPC title