Method for producing sulfide solid electrolyte, sulfide solid electrolyte, all-solid-state battery, and method for selecting raw material compound for use in producing sulfide solid electrolyte

Patent metadata

Field	Value
Publication number	US-2021194050-A1
Application number	US-201917270762-A
Country	US
Kind code	A1
Filing date	Aug 30, 2019
Priority date	Aug 30, 2018
Publication date	Jun 24, 2021
Grant date	—

Abstract

A method for producing a sulfide solid electrolyte according to an embodiment of the present invention is a method for producing a sulfide solid electrolyte, including: preparing a composition containing P, S, N, an element A, and an element M; reacting the composition to obtain an intermediate; and heating the intermediate to obtain a sulfide solid electrolyte, where the composition includes a raw material compound containing N, the element A, and the element M. A represents at least one element selected from the group consisting of Li, Na, and K. M represents at least one element selected from the group consisting of Al, Ta, Si, Sc, Mg, Nb, B, Hf, C, P, Zr, and Ti.

First claim

1 . A method for producing a sulfide solid electrolyte, the method comprising:
preparing a composition containing P, S, N, an element A, and an element M; reacting the composition to obtain an intermediate; and heating the intermediate to obtain a sulfide solid electrolyte, wherein the composition includes a raw material compound containing N, the element A, and the element M (A represents at least one element selected from the group consisting of Li, Na, and K; M represents at least one element selected from the group consisting of Al, Ta, Si, Sc, Mg, Nb, B, Hf, C, P, Zr, and Ti).

2 . The method for producing a sulfide solid electrolyte according to claim 1 , the method further comprising reacting a nitride of the element M and a nitride of the element A to obtain the raw material compound containing N, the element A, and the element M.

3 . The method for producing a sulfide solid electrolyte according to claim 1 , wherein the element M is at least one element selected from the group consisting of Al, Ta, Si, Sc, Mg, Nb, and B.

4 . The method for producing a sulfide solid electrolyte according to claim 1 , wherein the composition includes a lithium sulfide, a phosphorus sulfide, and the raw material compound containing N, the element A, and the element M.

5 . The method for producing a sulfide solid electrolyte according to claim 1 , wherein
the element A contains Li, a content ratio of Li to P in the composition is 2.30 or more and 4.20 or less in terms of mole ratio, and a content ratio of N to P in the composition is 0.0100 or more and 1.20 or less in terms of mole ratio.

6 . The method for producing a sulfide solid electrolyte according to claim 1 , wherein
the element A contains Li, a content ratio of Li to P in the composition is 2.77 or more and 3.38 or less in terms of mole ratio, and a content ratio of N to P in the composition is 0.280 or more and 0.650 or less in terms of mole ratio.

7 . The method for producing a sulfide solid electrolyte according to claim 1 , wherein the composition contains an element X
(X represents at least one element selected from the group consisting of Cl, Br, and I).

8 . The method for producing a sulfide solid electrolyte according to claim 7 , wherein
a content ratio of Li to P in the composition is 3.10 or more and 4.20 or less in terms of mole ratio, a content ratio of N to P in the composition is 0.0600 or more and 0.750 or less in terms of mole ratio, and a content ratio of X to P in the composition is 0.180 or more and 1.30 or less in terms of mole ratio.

9 . A sulfide solid electrolyte produced by the production method according to claim 1 .

10 . A method for selecting a raw material compound for use in producing a sulfide solid electrolyte, the method comprising:
selecting a candidate material containing N, an element A′, and an element M′ as a candidate for the raw material compound; and using a first principle calculation to calculate defect generation energy E Ndefect of N inside the candidate material, wherein the candidate material is selected as the raw material compound when the E Ndefect is 4.00 eV or more.

11 . The method for selecting a raw material compound for use in producing a sulfide solid electrolyte according to claim 10 , wherein the candidate material is selected as the raw material compound when the E Ndefect is 4.10 eV or more.

12 . The method for selecting a raw material compound according to claim 10 , wherein the candidate material is selected as the raw material compound when the E Ndefect is 4.35 eV or more.

13 . A method for producing a sulfide solid electrolyte, the method comprising:
preparing a composition including a raw material compound selected by the method for selecting a raw material compound for use in producing a sulfide solid electrolyte according to claim 10 ; reacting the composition to obtain an intermediate; and heating the intermediate to obtain a sulfide solid electrolyte.

14 . A sulfide solid electrolyte produced by the production method according to claim 13 .

15 - 18 . (canceled)

19 . A crystalline sulfide solid electrolyte comprising P, S, N, an element A, and an element M, and having crystallinity
(A represents at least one element selected from the group consisting of Li, Na, and K; M represents at least one element selected from the group consisting of Al, Ta, Si, Sc, Mg, Nb, B, Hf, C, P, Zr, and Ti).

20 . The sulfide solid electrolyte according to claim 19 , wherein the element M is at least one element selected from the group consisting of Al, Ta, Si, Sc, Mg, Nb, and B.

21 . The sulfide solid electrolyte according to claim 19 , further comprising an element X,
(X represents at least one element selected from the group consisting of Cl, Br, and I).

22 . The sulfide solid electrolyte according to claim 21 , wherein the crystalline structure has diffraction peaks at 2θ=20.2°±0.5° and 23.6°±0.5° in X-ray diffraction measurement with a CuKα line.

23 . An all-solid-state battery comprising the sulfide solid electrolyte according to claim 9 .

24 . An all-solid-state battery comprising the sulfide solid electrolyte according to claim 19 .

Assignees

• Gs Yuasa Int Ltd

Inventors

• Fukushima Akihiro
• Nishii Katsuya
• Sakuma Ryo
• Kakeya Tadashi
• Ochi Ryuya

Classifications

• H01M2004/027

  Negative electrodes · CPC title

• H01M4/62

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

• H01M4/13

  Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof · CPC title

• H01M10/0562 Primary

  Solid materials · CPC title

• H01M2300/0068

  inorganic · CPC title