Sodium-conducting solid electrolyte

Patent metadata

Field	Value
Publication number	US-9966629-B2
Application number	US-201514698691-A
Country	US
Kind code	B2
Filing date	Apr 28, 2015
Priority date	Feb 3, 2015
Publication date	May 8, 2018
Grant date	May 8, 2018

Abstract

A sodium-conductive solid-state electrolyte material includes a compound of the composition Na 10 MP 2 S 12 , wherein M is selected from Ge, Si, and Sn. The material may have a conductivity of at least 1.0×10 −5 S/cm at a temperature of about 300K and may have a tetragonal microstructure, e.g., a skewed P1 crystallographic structure. Also provided are an electrochemical cell that includes the sodium-conductive solid-state electrolyte material and a method for producing the sodium-conductive solid electrolyte material via controlled thermal processing parameters.

First claim

We claim:

1. A sodium-conductive solid-state electrolyte material comprising a compound of the composition Na 10 MP 2 S 12 , wherein M is selected from Ge, Si, and Sn.

2. The electrolyte material of claim 1 , wherein M is Ge.

3. The electrolyte material of claim 1 , wherein M is Si.

4. The electrolyte material of claim 1 , wherein M is Sn.

5. The electrolyte material of claim 1 , having a conductivity of at least 1.0×10 −5 S/cm at a temperature of 300K.

6. The electrolyte material of claim 5 , wherein the conductivity is at least 1.0×10 −4 S/cm at a temperature of 300K.

7. The electrolyte material of claim 1 , having a peak in positions of within 0.50° of 2θ=18.18°, 26.74°, 33.88°, 36.90°, 38.07°, 42.59°, and/or 46.10° as measured by X-ray diffraction using CuKα radiation.

8. The electrolyte material of claim 1 , having a tetragonal structure.

9. The electrolyte material of claim 8 , wherein the tetragonal structure is a skewed P1 structure.

10. The electrolyte material of claim 1 , consisting essentially of Na 10 MP 2 S 12 , wherein M is selected from Ge, Si, and Sn.

11. An electrochemical cell comprising:
an anode layer containing an anode material;
a cathode layer containing a cathode material; and
an electrolyte layer between the anode and cathode layers,
wherein a solid-state, Na-conductive material is present in the cathode layer, the electrolyte layer, or both, the material comprising a compound of the composition Na 10 MP 2 S 12 , M being selected from Ge, Si, and Sn.

12. The electrochemical cell of claim 11 , wherein the cell is a solid-state cell.

13. The electrochemical cell of claim 11 , wherein the cell is rechargeable.

14. A method for producing a sodium-conductive solid electrolyte material, comprising:
forming a raw material composition from elements Na, P, S, and M, wherein element M is selected from Ge, Si, and Sn;
heating the raw material composition to a temperature effective to form a solution; and
cooling the solution at a rate no greater than 1° C. per minute to produce the electrolyte material,
wherein the electrolyte material exhibits an conductivity of at least 1.0×10 −4 S/cm at a temperature at 300K and the method is carried out within no more than 200 hours.

15. The method of claim 14 , wherein the plurality of compounds includes Na 2 S, P 2 S 5 , and MS 2 , wherein M is selected from Ge, Si, and Sn.

16. The method of claim 14 , further comprising heating the raw material composition to a melting temperature before cooling.

17. The method of claim 14 , further comprising heating the raw material composition to a peak temperature of at least about 350° C. for at least 2 hours.

18. The method of claim 17 , further comprising heating the raw material composition to a peak temperature of at least 550° C.

19. The method of claim 18 , further comprising heating the raw material composition to 700° C.

20. The method of claim 14 , wherein the solution is cooled at a rate no greater than 0.5° C. per minute.

21. The method of claim 14 , wherein the solid-state solution is cooled at a rate no greater than 0.2° C. per minute.

22. The method of claim 14 , wherein the solid-state solution is cooled at a rate no greater than 0.1° C. per minute.

Assignees

• Samsung Electronics Co Ltd
• Massachusetts Inst Technology
• Samsung Electronics Co Ltd

Inventors

• Richards William D
• Ong Shyue Ping
• Mo Yifei
• Ceder Gerbrand
• Miara Lincoln
• Tsujimura Tomoyuki
• Wang Yan
• Ryu Young-Gyoon
• Suzuki Naoki
• Uechi Ichiro

Classifications

• C01B25/14

  Sulfur, selenium, or tellurium compounds of phosphorus · CPC title

• H01M10/05

  Accumulators with non-aqueous electrolyte (H01M10/39 takes precedence) · CPC title

• C01P2002/72

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

• H01M10/0562 Primary

  Solid materials · CPC title

• H01M4/381

  Alkaline or alkaline earth metals elements (H01M4/40 takes precedence) · CPC title