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

Patent metadata

Field	Value
Publication number	US-2018016185-A1
Application number	US-201515522580-A
Country	US
Kind code	A1
Filing date	Oct 30, 2015
Priority date	Oct 31, 2014
Publication date	Jan 18, 2018
Grant date	—

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

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 - 8 . (canceled)

9 . Sulfide glass satisfying a formula (9):
Tc 1+45≦ Tc 2   (9)
wherein in the formula, Tc1 is the temperature of an exothermic peak that appears for the first time when sulfide glass is subjected to differential thermogravimetry in a dry nitrogen atmosphere at a temperature-elevating rate of 10° C./min from 20° C. to 600° C., and Tc2 is the temperature of an exothermic peak that appears subsequent to the appearance of an exothermic peak of which the temperature is Tc1.

10 - 19 . (canceled)

20 . 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.

21 . 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.

22 . 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.

23 . The method of claim 20 , 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.

24 . The method of claim 1 , wherein the phosphorus sulfide further satisfies formulas (3) and (6):
37≦100× A/B≦ 10   (3)
0.1≦100× A/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.

25 . 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.

26 . The method of claim 25 , wherein the raw material further comprises a lithium halide.

27 . The method of claim 26 , wherein the raw material is mixed in a solvent.

28 . The method of claim 27 , wherein the solvent is a hydrocarbon solvent.

29 . 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.

30 . The method of claim 20 , wherein the raw material further comprises lithium sulfide and a lithium halide.

31 . The method of claim 30 , wherein the raw material is mixed in a solvent.

32 . 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.

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

34 . The method of claim 33 , wherein the raw material further comprises a lithium halide.

35 . The method of claim 34 , 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.

36 . The sulfide glass according to claim 9 , comprising Li, P, S and a halogen.

Assignees

• Idemitsu Kosan Co

Inventors

• Nakata Akiko
• Maruyama Junpei

Classifications

• H01B13/00

  Apparatus or processes specially adapted for manufacturing conductors or cables · CPC title

• H01M4/587

  for inserting or intercalating light metals · CPC title

• C03C3/32 Primary

  Non-oxide glass compositions, e.g. binary or ternary halides, sulfides or nitrides of germanium, selenium or tellurium · CPC title

• H01M4/62

  Selection of inactive substances as ingredients for active masses, e.g. binders, fillers · CPC title

• H01B1/10

  sulfides · CPC title