Lithium ion conductive sulfide-based solid electrolyte comprising indium selenide and a method for preparing the same

Patent metadata

Field	Value
Publication number	US-10790540-B2
Application number	US-201815994269-A
Country	US
Kind code	B2
Filing date	May 31, 2018
Priority date	Aug 8, 2017
Publication date	Sep 29, 2020
Grant date	Sep 29, 2020

Abstract

The present invention relates to a lithium-ion-conductive sulfide-based solid electrolyte which contains lithium (Li), sulfur (S), phosphorus (P), indium (In) and selenium (Se) and has a crystal structure of InSe and a method for preparing the same.

First claim

What is claimed is:

1. A lithium-ion-conductive sulfide-based solid electrolyte comprising:
lithium (Li);
sulfur (S);
phosphorus (P);
indium (In); and
selenium (Se),
wherein said Li, S, P, In and Se of the electrolyte are represented by the following formula:
(Li 2 S) a .(P 2 S 5 ) b .(In 2 Se 3 ) c ,

wherein 0.5≤a≤0.8, 0.1≤b≤0.4, 0.01≤c≤0.3, and a+b+c=1.

2. The lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 , which has a crystal structure of InSe.

3. The lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 , which shows XRD peaks of InSe at 2θ=20-22°, 2θ=26-28°, 2θ=38-40° and 2θ=44-46° when subjected to X-ray diffraction (XRD) pattern measurement using Cu Kα radiation.

4. The lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 , wherein 0.65≤a≤0.8, 0.15≤b≤0.25 and 0.02≤c≤0.2.

5. The lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 , which has an ion conductivity after exposure to the atmosphere of 40% or greater with respect to an ion conductivity before exposure to the atmosphere, wherein the exposure to the atmosphere means exposure of the sulfide-based solid electrolyte to a condition of 20-25° C. and 50-70% humidity for 30 minutes to 3 hours.

6. The lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 , which further comprises an element selected from a group consisting of boron (B), carbon (C), nitrogen (N), aluminum (Al), silicon (Si), vanadium (V), manganese (Mn), iron (Fe), cobalt (Co), nickel (Ni), copper (Cu), zinc (Zn), gallium (Ga), germanium (Ge), arsenic (As), silver (Ag), cadmium (Cd), tin (Sn), antimony (Sb), tellurium (Te), lead (Pb), bismuth (Bi) and a combination thereof.

7. A method for preparing a lithium-ion-conductive sulfide-based solid electrolyte, comprising:
mixing lithium sulfide (Li 2 S), a sulfide-based raw material and indium selenide (In 2 Se 3 ); and
milling the resulting mixture, and
wherein the lithium-ion-conductive sulfide-based solid electrolyte is represented by the following formula:
(Li 2 S) a .(P 2 S 5 ) b .(In 2 Se 3 ) c ,

wherein 0.5≤a≤0.8, 0.1≤b≤0.4, 0.01≤c≤0.3, and a+b+c=1.

8. The method for preparing a lithium-ion-conductive sulfide-based solid electrolyte according to claim 7 , wherein the sulfide-based raw material is selected from a group consisting of P 2 S 3 , P 2 S 5 , P 4 S 3 , P 4 S 5 , P 4 S 7 , P 4 S 10 and a combination thereof.

9. The method for preparing a lithium-ion-conductive sulfide-based solid electrolyte according to claim 7 , wherein the lithium sulfide (Li 2 S), the indium selenide (In 2 Se 3 ), and phosphorus pentasulfide (P 2 S 5 ) are mixed.

10. The method for preparing a lithium-ion-conductive sulfide-based solid electrolyte according to claim 7 , which further comprises heat-treating the milled mixture.

11. The method for preparing a lithium-ion-conductive sulfide-based solid electrolyte according to claim 10 , wherein the heat-treating is performed at 200-1200° C. for 1-3 hours.

12. An all-solid-state battery comprising:
an anode;
a cathode; and
an electrolyte layer interposed between the anode and the cathode,
wherein one or more of the anode, the cathode and the electrolyte layer comprises the lithium-ion-conductive sulfide-based solid electrolyte according to claim 1 .

Assignees

• Korea Inst Sci & Tech

Inventors

• Kim Hyoungchul
• Lee Hae-Weon
• Kim Byung Kook
• Lee Jong Ho
• Son Ji-Won
• Jung Hun-Gi
• Jung Eu Deum
• Choi Sung Jun
• Yoon Bin Na

Classifications

• H01M10/052

  Li-accumulators · CPC title

• H01M2300/0068

  inorganic · CPC title

• H01M2004/027

  Negative electrodes · CPC title

• C01B17/22

  Alkali metal sulfides or polysulfides · CPC title

• H01B1/10

  sulfides · CPC title