Sulfide glass and crystalline solid electrolyte production method, crystalline solid electrolyte, sulfide glass and solid-state battery

Patent metadata

Field	Value
Publication number	US-10280109-B2
Application number	US-201515522580-A
Country	US
Kind code	B2
Filing date	Oct 30, 2015
Priority date	Oct 31, 2014
Publication date	May 7, 2019
Grant date	May 7, 2019

Abstract

A method for producing sulfide glass wherein phosphorus sulfide satisfying the following formula (1) is used as a raw material:

100× A/B ≥37  (1)

wherein in the formula, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

First claim

The invention claimed is:

1. A method comprising producing sulfide glass from a raw material comprising phosphorus sulfide satisfying a formula (1):
100× A/B≥ 37  (1)

wherein in the formula, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

2. A method comprising producing sulfide glass from a raw material comprising phosphorus sulfide satisfying a formula (2):
37≤100×( A+D )/ B ≤70  (2)

wherein in the formula, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, D is peak areas of peaks that appear at peak positions in a range of 84.0 ppm or more and 86.0 ppm or less, and 110 ppm or more and 113 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

3. The method of claim 1 , wherein the phosphorus sulfide further satisfies a formula (2):
37≤100×( A+D )/ B ≤70  (2)

wherein in the formula, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, D is peak areas of peaks that appear at peak positions in a range of 84.0 ppm or more and 86.0 ppm or less, and 110 ppm or more and 113 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

4. The method of claim 1 , wherein the phosphorus sulfide further satisfies formulas (3) and (4):
37≤100× A/B≤ 60  (3)

25≤100× C/B≤ 60  (4)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, C is peak areas of peaks that appear in a range of 56.6 ppm or more and 57.1 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

5. The method of claim 1 , wherein the phosphorus sulfide further satisfies formulas (3), (4) and (5):
37≤100× A/B≤ 60  (3)

25≤100× C/B≤ 60  (4)

0≤100× D/B≤ 10  (5)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, C is peak areas of peaks that appear in a range of 56.6 ppm or more and 57.1 ppm or less in 31 PNMR spectroscopy, and D is peak areas of peaks that appear in a range of 84.0 ppm or more and 86.0 ppm or less, and 110 ppm or more and 113 ppm or less, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

6. The method of claim 3 , wherein the phosphorus sulfide further satisfies formulas (3), (4) and (5):
37≤100× A/B≤ 60  (3)

25≤100× C/B≤ 60  (4)

0≤100× D/B≤ 10  (5)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, C is peak areas of peaks that appear in a range of 56.6 ppm or more and 57.1 ppm or less in 31 PNMR spectroscopy, and D is peak areas of peaks that appear in a range of 84.0 ppm or more and 86.0 ppm or less, and 110 ppm or more and 113 ppm or less, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

7. The method of claim 1 , wherein the phosphorus sulfide further satisfies formulas (3) and (6):
37≤100× A/B≤ 60  (3)

0.1≤100× D/B≤ 10  (6)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, D is peak areas of peaks that appear in a range of 84.0 ppm or more and 86.0 ppm or less, and 110 ppm or more and 113 ppm or less, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

8. The method of claim 1 , wherein the phosphorus sulfide further satisfies a formula (3), and the raw material further comprises lithium sulfide:
37≤100× A/B≤ 60  (3)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

9. The method of claim 8 , wherein the raw material further comprises a lithium halide.

10. The method of claim 9 , wherein the raw material is mixed in a solvent.

11. The method of claim 10 , wherein the solvent is a hydrocarbon solvent.

12. The method of claim 1 , wherein the phosphorus sulfide further satisfies a formula (3), and the raw material is mixed in a solvent:
37≤100× A/B≤ 60  (3)

wherein in the formulas, A is peak areas of peaks that appear at peak positions in a range of 57.2 ppm or more and 58.3 ppm or less, and 63.0 ppm or more and 64.5 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

13. The method of claim 3 , wherein the raw material further comprises lithium sulfide and a lithium halide.

14. The method of claim 13 , wherein the raw material is mixed in a solvent.

15. The method of claim 2 , wherein the phosphorus sulfide further satisfies formula (4):
25≤100× C/B≤ 60  (4)

wherein in the formula, C is peak areas of peaks that appear in a range of 56.6 ppm or more and 57.1 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

16. The method of claim 2 , wherein the raw material further comprises lithium sulfide.

17. The method of claim 16 , wherein the raw material further comprises a lithium halide.

18. The method of claim 17 , wherein the phosphorus sulfide further satisfies formula (4):
25≤100× C/B≤ 60  (4)

wherein in the formula, C is peak areas of peaks that appear in a range of 56.6 ppm or more and 57.1 ppm or less in 31 PNMR spectroscopy, and B is the total of peak areas of all peaks measured in 31 PNMR spectroscopy.

Assignees

• Idemitsu Kosan Co

Inventors

• Nakata Akiko
• Maruyama Junpei

Classifications

• C03C3/321

  Chalcogenide glasses, e.g. containing S, Se, Te · CPC title

• C03C1/02

  Pretreated ingredients · CPC title

• H01M2300/008

  Halides · CPC title

• C03C4/14

  for electro-conductive glass · CPC title

• H01M10/0562

  Solid materials · CPC title