# US 12,119,443 B2 · Solid-state electrolyte, solid-state battery including the electrolyte, and method of making the same

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- Number: US 12,119,443 B2
- Document ID: US12119443B2
- Status: Granted
- Kind: B2
- Application number: 18/119,927
- Filed: 2023-03-10
- Published: 2023-08-17
- Granted: 2024-10-15
- Earliest claimed: 2020-11-25
- Assignees: Samsung Electronics Co., Ltd.
- Applicants: Samsung Electronics Co., Ltd.
- Inventors: Yan Wang; Lincoln Miara
- Web page: https://patentgrep.com/patent/US12119443B2

## CPC

- H01M 10/052: Li-accumulators
- H01M 10/0562: Solid materials
- H01M 4/0471: {involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis}
- H01M 4/131: Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/1391: of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/1395: of electrodes based on metals, Si or alloys
- H01M 4/364: {as mixtures}
- H01M 4/661: {Metal or alloys, e.g. alloy coatings (H01M4/669 take precedence)}
- H01M 4/667: {in the form of layers, e.g. coatings}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 2004/027: {Negative electrodes}
- H01M 2004/028: {Positive electrodes}
- H01M 2300/0071: Oxides
- Y02E 60/10: Energy storage using batteries
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A solid-state ion conductor includes a compound of Formula 1: Li16+(5−n)*a−(2+m)*bM2−aXnaN8O1−bAmb Formula 1 wherein, in Formula 1, M is Ta, Nb, V, or a combination thereof, X is an element having an oxidation state of n, wherein n is +1, +2, +3, +4, or a combination thereof, A is an element having an oxidation state of m, wherein m is −1, −2, or a combination thereof, and 0<a≤2 and 0≤b≤1.

## Claims

### Claim 1

A solid-state ion conductor comprising a compound of Formula 1:
Li16+(5−n)*a−(2+m)*bM2−aXnaN8O1−bAmb Formula 1
wherein, in Formula 1,
M is Ta, Nb, V, or a combination thereof,
X is an element having an oxidation state of n, wherein n is +1, +2, +3, or +4,
A is an element having an oxidation state of m, wherein m is −1, −2, or a combination thereof, and
0<a<2 and 0≤b≤1.

### Claim 2 (depends on 1)

The solid-state ion conductor of claim 1, wherein M comprises Ta.

### Claim 3 (depends on 2)

The solid state ion conductor of claim 2, wherein the solid-state ion conductor comprises Li49Ta5HfN24O3, Li50Ta4Hf2N24O3, Li51Ta3Hf3N24O3, Li52Ta2Hf4N24O3, Li53TaHf5N24O3, Li17TaGeN8O, Li17TaZrN8O, Li17TaTiN8O, Li17TaSnN8O, Li17TaSiN8O, Li18TaGaN8O, Li18TaLaN8O, Li18TaYN8O, Li18TaScN8O, Li18TaInN8O, Li18TaAlN8O, Li17TaGeN8O, Li17TaZrN8O, La17TaTiN8O, Li17TaSnN8O, or Li17TaSiN8O.

### Claim 4 (depends on 1)

The solid-state ion conductor of claim 1, wherein X is Hf, Zr, Ti, Ge, Sn, Si, Ga, La, Y, Sc, In, Al, Ca, Ba, Mg, Na, K, or a combination thereof.

### Claim 5 (depends on 1)

The solid-state ion conductor of claim 1, wherein X is Hf, Zr, Ti, Si, or a combination thereof.

### Claim 6 (depends on 1)

The solid-state ion conductor of claim 1,
wherein n is +3 and X is Ga, La, Y, Sc, In, Al, or a combination thereof; or
wherein n is +4 and X is Ge, Zr, Ti, Sn, Si, or a combination thereof.

### Claim 7 (depends on 1)

The solid-state ion conductor of claim 1, wherein A is F, Cl, Br, S, Se, or a combination thereof.

### Claim 8 (depends on 1)

The solid-state ion conductor of claim 1, wherein 0<a≤0.5.

### Claim 9 (depends on 1)

The solid-state ion conductor of claim 1, wherein 0<a≤0.25.

### Claim 10 (depends on 1)

The solid-state ion conductor of claim 1, wherein b=0.

### Claim 11 (depends on 1)

The solid-state ion conductor of claim 1, having an ionic conductivity of greater than 1×10−7 Siemens per centimeter at room temperature.

### Claim 12 (depends on 11)

The solid-state ion conductor of claim 11, having an ionic conductivity of 1×10−6 to 1×10−2 Siemens per centimeter at room temperature.

### Claim 13 (depends on 1)

A component of a lithium secondary electrochemical cell comprising:
a current collector; and
the solid-state ion conductor of claim 1 on the current collector.

### Claim 14 (depends on 13)

The component of claim 13, wherein the current collector comprises at least one of nickel, copper, titanium, stainless steel, or amorphous carbon and/or wherein the solid-state ion conductor is in a form of a layer on the current collector.

### Claim 15 (depends on 1)

A negative electrode comprising:
a negative active material comprising lithium metal, a lithium metal alloy, or combination thereof; and
the solid-state ion conductor of claim 1 on the negative active material.

### Claim 16 (depends on 1)

A separator for a lithium battery comprising:
a substrate; and
the solid-state ion conductor of claim 1 disposed on a surface of the substrate.

### Claim 17 (depends on 1)

An electrochemical cell comprising:
a positive electrode;
a negative electrode; and
an electrolyte between the positive electrode and the negative electrode, wherein at least one of the negative electrode or the electrolyte comprise the solid-state ion conductor of claim 1.

### Claim 18 (depends on 17)

The electrochemical cell of claim 17,
wherein the negative electrode comprises lithium metal, a lithium metal alloy, or combination thereof, and
wherein the solid-state ion conductor is between the positive electrode and the negative electrode.

### Claim 19 (depends on 18)

The electrochemical cell of claim 18, wherein the compound of Formula 1 is directly on the negative electrode.

### Claim 20 (depends on 1)

A method of preparing the compound of claim 1, the method comprising:
contacting a lithium compound, a compound comprising Ta, Nb, V, or a combination thereof, a compound comprising an element having an oxidation state of +1, +2, +3, +4, or a combination thereof, and a compound comprising an element having an oxidation state of −1, −2, or a combination thereof to provide a mixture; and
treating the mixture to prepare the compound.

### Claim 21 (depends on 20)

The method of claim 20, wherein treating the mixture comprises mechanochemical milling of the mixture to prepare a compound of Formula 1.

### Claim 22 (depends on 21)

The method of claim 21, wherein the treating is heat-treating the mixture at 25° C. to 800° C. to prepare the compound of Formula 1.

### Claim 23 (depends on 1)

A method of manufacturing an electrochemical cell, the method comprising:
providing a negative electrode comprising lithium, a lithium alloy, or combination thereof;
disposing the solid-state ion conductor of claim 1 on the negative electrode;
disposing an electrolyte on the negative electrode; and
disposing a positive electrode on the electrolyte to manufacture the electrochemical cell.

### Claim 24

A solid-state ion conductor comprising a compound of Formula 1:
Li16+(5−n)*a−(2+m)*bM2−aXnaN8O1−bAmb Formula 1
wherein, in Formula 1,
M is Ta, Nb, V, or a combination thereof,
X is an element having an oxidation state of n, wherein n is +1, +2, +3, or +4,
A is an element having an oxidation state of m, wherein m is −1, −2, or a combination thereof, and wherein A is F, Cl, Br, S, Se, or a combination thereof, and
0≤a<2 and 0<b≤1.

### Claim 25 (depends on 24)

A component of a lithium secondary electrochemical cell comprising:
a current collector; and
the solid-state ion conductor of claim 24 on the current collector.

### Claim 26 (depends on 24)

A negative electrode comprising:
a negative active material comprising lithium metal, a lithium metal alloy, or combination thereof; and
the solid-state ion conductor of claim 24 on the negative active material.

### Claim 27 (depends on 24)

A separator for a lithium battery comprising:
a substrate; and
the solid-state ion conductor of claim 24 disposed on a surface of the substrate.

### Claim 28 (depends on 24)

An electrochemical cell comprising:
a positive electrode;
a negative electrode; and
an electrolyte between the positive electrode and the negative electrode, wherein at least one of the negative electrode or the electrolyte comprise the solid-state ion conductor of claim 24.