# US 10,770,751 B2 · Solid state lithium-ion conductor

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- Number: US 10,770,751 B2
- Document ID: US10770751B2
- Status: Granted
- Kind: B2
- Application number: 16/205,715
- Filed: 2018-11-30
- Published: 2019-11-21
- Granted: 2020-09-08
- Earliest claimed: 2018-05-17
- Assignees: Samsung Electronics Co., Ltd.
- Applicants: Samsung Electronics Co., Ltd.
- Inventors: Yan Wang; Lincoln Miara
- Web page: https://patentgrep.com/patent/US10770751B2

## CPC

- C01G 27/00: Compounds of hafnium
- H01M 10/0562: Solid materials
- C01G 25/006: {Compounds containing zirconium, with or without oxygen or hydrogen, and containing two or more other elements}
- C01G 27/006: {Compounds containing hafnium, with or without oxygen or hydrogen, and containing two or more other elements}
- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/366: {as layered products}
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 4/405: {Alloys based on lithium}
- H01M 4/628: {Inhibitors, e.g. gassing inhibitors, corrosion inhibitors}
- H01M 10/052: Li-accumulators
- C01P 2002/54: one element only
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2002/77: by unit-cell parameters, atom positions or structure diagrams
- C01P 2006/40: Electric properties
- H01M 2004/027: {Negative electrodes}
- H01M 2300/0071: Oxides
- Y02E 60/10: Energy storage using batteries
- C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A compound of Formula 1: Li6+(4−a)x+c)M4+(2−x)Aa+xO(7−c)N′c (1) wherein M is a tetravalent cationic element, A is a divalent or trivalent cationic element, N′ is an anion having a valence of less than −2, wherein when A is Y3+, In3+, Zn2+, or a combination thereof, 0.15<x≤0.5, otherwise 0≤x≤0.5, 0≤c≤2, and ((4−a)x+c)>0.

## Claims

### Claim 1

A compound of Formula 1 in a positive electrode, negative electrode or electrolyte, comprising:
Li(6+(4−a)x+c)M4+(2−x)Aa+xO(7−c)N′c (1)
wherein
M is a tetravalent cationic element,
A is a divalent or trivalent cationic element,
N′ is an anion Group 15 element,
wherein when A is Y3+, In3+, Zn2−, or a combination thereof, 0.15<x≤0.5, otherwise
0≤x≤0.5, 0≤c≤2, and
((4−a)x+c)>0.

### Claim 2 (depends on 1)

The compound of claim 1, wherein M comprises an element of Group 4, Group 14, or a combination thereof.

### Claim 3 (depends on 2)

The compound of claim 2, wherein M is Zr, Hf, or a combination thereof.

### Claim 4 (depends on 1)

The compound of claim 1, wherein A comprises Mg, Ca, Zn, or a combination thereof.

### Claim 5 (depends on 1)

The compound of claim 1, wherein A comprises Y, Gd, Ga, In, Al, La, Sc, or a combination thereof.

### Claim 6 (depends on 1)

The compound of claim 1, wherein N′ is N.

### Claim 7 (depends on 1)

The compound of claim 1, wherein 0.1≤((4−a)x+c)≤0.4.

### Claim 8 (depends on 1)

The compound of claim 1, wherein the compound is of Formula 2:
Li(6+2a′−a″+c)M(2−(a′+a″))A′a′A″a″O7−cN′c (2)
wherein
M comprises Zr, Hf, or a combination thereof,
A′ is a divalent cationic element,
A″ is a trivalent cationic element,
N′ is an anion having a valence of less than −2,
wherein when A′ is Zn, 0.15<a′≤0.5, or when A″ is Y or In, 0.15<a″≤0.5, otherwise
0≤a′≤0.5, 0≤a″≤0.5, 0≤c≤1, and
(a′+a″+c)>0.

### Claim 9 (depends on 8)

The compound of claim 8, wherein A′ is Mg, A″ is Sc, and N′ is N, and
wherein 0.1<(2a′+a″+c)<0.3, 0<a′<0.15, 0≤a″<0.3, and 0≤c≤0.3.

### Claim 10 (depends on 1)

The compound of claim 1, having an ionic conductivity of greater than 1×10−7 Siemens per centimeter.

### Claim 11 (depends on 7)

The compound of claim 7, having an ionic conductivity of 1×10−6 to 1×10−2 Siemens per centimeter.

### Claim 12

A component of a lithium secondary electrochemical cell comprising the compound of Formula 1
Li(6+(4−a)x+c)M4+(2−x)Aa+xO(7−c)N′c (1)
wherein
M is a tetravalent cationic element,
A is a divalent or trivalent cationic element,
N′ is an anion of a Group 15 element,
wherein when A is Y3+, In3+, Zn2+, or a combination thereof, 0.15<x≤0.5, otherwise 0≤x≤0.5, 0≤c≤2, and ((4−a)x+c)>0.

### Claim 13 (depends on 9)

The component of claim 9, wherein the component is an electrolyte.

### Claim 14 (depends on 9)

The component of claim 9, wherein the component is in the form of a protection layer on a negative electrode comprising lithium metal, a lithium metal alloy, or combination thereof.

### Claim 15

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 positive electrode, the negative electrode and the electrolyte comprise the compound of Formula 1
Li(6+(4−a)x+c)M4+(2−x)Aa+xO(7−c)N′c (1)
wherein
M is a tetravalent cationic element,
A is a divalent or trivalent cationic element,
N′ is an anion of a Group 15 element, wherein when A is Y3+, In3+, Zn2+, or a combination thereof, 0.15<x≤0.5, otherwise 0≤x≤0.5, 0≤c≤2, and ((4−a)x+c)>0.

### Claim 16 (depends on 14)

The electrochemical cell of claim 14, wherein the negative electrode comprises lithium metal, a lithium metal alloy, or combination thereof, and wherein the compound of Formula 1 is directly on the negative electrode.

### Claim 17 (depends on 1)

A method of preparing the compound of claim 1, the method comprising:
contacting a lithium compound, a compound comprising a tetravalent cationic element, a compound comprising at least one of divalent cationic element and a trivalent cationic element to provide a mixture; and
heat-treating the mixture to prepare the compound.

### Claim 18

A method of manufacturing an electrochemical cell, the method comprising:
providing a negative electrode comprising lithium, a lithium alloy, or combination thereof;
disposing the compound of Formula 1 on the negative electrode;
disposing an electrolyte on the negative electrode; and
disposing a positive electrode on the separator to manufacture the electrochemical cell.