Solid electrolyte

Patent metadata

Field	Value
Publication number	US-9673482-B2
Application number	US-201314441051-A
Country	US
Kind code	B2
Filing date	Nov 5, 2013
Priority date	Nov 6, 2012
Publication date	Jun 6, 2017
Grant date	Jun 6, 2017

Abstract

A solid electrolyte glass at least including: at least one alkali metal element;
a phosphorus (P) element; a sulfur (S) element; and one or more halogen elements selected from I, Cl, Br and F; wherein the solid electrolyte glass has two exothermic peaks that are separated from each other in a temperature range of 150° C. to 350° C. as determined by differential scanning calorimetry (in a dry nitrogen atmosphere at a temperature-elevating speed of 10° C./min from 20 to 600° C.).

First claim

The invention claimed is:

1. A solid electrolyte glass having a composition represented by the formula (1′):
L a MP c S d X e O f
wherein:
L is an alkali metal;
M is one or more elements selected from the group consisting of B, Al, Si, Ge, As, Se, Sn, Sb, Te, Pb and Bi; and
X includes Br and optionally further includes and at least one element selected from the group consisting of I, Cl, and F, and
a to f independently satisfy:
0< a≦ 12,
0≦ b< 0.2

c= 1
0< d≦ 9,
0< e≦ 9, and
0< f≦ 9

wherein the solid electrolyte glass has two exothermic peaks that are separated from each other in a temperature range of 150° C. to 350° C. as determined by differential scanning calorimetric measurement (in a dry nitrogen atmosphere at a temperature-elevating speed of 10° C./min from 20° C. to 600° C.).

2. A method for producing the solid electrolyte glass according to claim 1 , the method comprising:
mixing raw materials (1-A), (1-B), (1-C), and (1-D):
(1-A) an alkali metal sulfide;
(1-B) a compound represented by M′ m S n ;
(1-C) a compound represented by M″ w X′ y ; and
(1-D) Li 2 SO 3 ,

to form the solid electrolyte glass according to claim 1 ,
wherein:
M′ is B, Al, Si, P or Ge;
M″ is Li, Na, B, Al, Si, P, S, Ge, As, Se, Sn, Sb, Te, Pb or Bi;
X′ is Br;
w is an integer of 1 to 2;
m, n and y are an integer of 1 to 10.

3. The method according to claim 2 , wherein the mixing of the raw materials comprises reacting the raw materials (1-A) and (1-B) to form a reaction product of the raw materials (1-A) and (1-B), and adding the raw material (1-C) to the reaction product such that the raw material (1-C) reacts with the reaction product.

4. The method according to claim 2 , wherein the mixing of the raw materials comprises reacting the raw materials in an atmosphere having an oxygen concentration of 19 to 21%.

5. A method for producing a solid electrolyte glass ceramic, comprising:
subjecting the solid electrolyte glass according to claim 1 to a heat treatment at a temperature between the two exothermic peaks.

6. The method according to claim 5 , wherein the solid electrolyte glass ceramic has an ionic conductivity of 1×10 −3 S/cm or more.

7. The method according to claim 2 , wherein the difference in temperature between the peak top positions of the two exothermic peaks is 20° C. or higher and 100° C. or lower.

8. The method according to claim 2 , wherein the raw material (1-A) is lithium sulfide or sodium sulfide.

9. The method according to claim 2 , wherein the raw material (1-B) is at least one selected from the group consisting of P 2 S 3 (phosphorus trisulfide), P 2 S 5 (phosphorus pentasulfide), SiS 2 (silicon sulfide), Al 2 S 3 (aluminum sulfide), GeS 2 (germanium sulfide), and B 2 S 3 (arsenic trisulfide).

10. The method according to claim 2 , wherein the raw material (1-C) is LiBr.

11. The method according to claim 2 , wherein:
when M″ in the component (1-C) is an element other than phosphorus, the molar ratio of component (1-A):component (1-B) is 65:35 to 85:15, and the ratio of the molar amount of (1-C) relative to the total of the molar amounts of the components (1-A) and (1-B) is 50:50 to 99:1; and
when M″ in the component (1-C) is phosphorus, the molar ratio of component (1-A):component (1-B) is 60:40 to 90:10, and the ratio of the molar amount of (1-C) relative to the total of the molar amounts of the components (1-A) and (1-B) is 50:50 to 99:1.

12. The solid electrolyte glass according to claim 1 , wherein the difference in temperature between the peak top positions of the two exothermic peak is 20° C. or higher and 100° C. or lower.

13. A solid electrolyte glass having a composition represented by the formula (1′):
L a P c S d X e O f
having two exothermic peaks that are separated from each other in a temperature range of 150° C. to 350° C. as determined by differential scanning calorimetric measurement (in a dry nitrogen atmosphere at a temperature-elevating speed of 10° C./min from 20° C. to 600° C.),
wherein:
the difference in temperature between the peak top positions of the two exothermic peak is 20° C. or higher and 100° C. or lower,
L is an alkali metal;
X includes Br and optionally further includes and least one element selected from the group consisting of I, Cl, and F, and
a, c, d and f indecently satisfy
0< a≦ 12,
c= 1
0< d≦ 9,
0< e≦ 9, and
0< f≦ 9.

Assignees

• Idemitsu Kosan Co

Inventors

• Kambara Takayoshi
• Higuchi Hiroyuki
• Tamura Hiroyuki
• Nakagawa Masaru
• Junke Tadanori

Classifications

• H01M2220/30

  Batteries in portable systems, e.g. mobile phone, laptop · CPC title

• C03C4/14

  for electro-conductive glass · CPC title

• C03C10/0072

  having a ferro-electric crystal phase · CPC title

• C03C3/321

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

• Y02P70/54

  Cross-Sectional Technologies · mapped topic