# US 2021/0083318 A1 · LITHIUM POTASSIUM TANTALATE COMPOUNDS AS Li SUPER-IONIC CONDUCTOR, SOLID ELECTROLYTE AND COATING LAYER FOR LITHIUM METAL BATTERY AND LITHIUM-ION BATTERY

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- Number: US 2021/0083318 A1
- Document ID: US20210083318A1
- Status: Published application
- Kind: A1
- Application number: 16/570,811
- Filed: 2019-09-13
- Published: 2021-03-18
- Earliest claimed: 2019-09-13
- Assignees: University of Maryland, College Park; Toyota Motor Engineering & Manufacturing North America, Inc.
- Applicants: University of Maryland, College Park; Toyota Motor Engineering & Manufacturing North America, Inc.
- Inventors: Yifei MO; Qiang BAI; Xingfeng HE; Chen LING
- Web page: https://patentgrep.com/patent/US20210083318A1

## CPC

- H01M 10/0562: Solid materials
- H01M 4/366: {as layered products}
- H01M 4/62: Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M 10/052: Li-accumulators
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01G 35/006: {Compounds containing tantalum, with or without oxygen or hydrogen, and containing two or more other elements}
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 2004/027: {Negative electrodes}
- H01M 2004/028: {Positive electrodes}
- H01M 2300/0068: inorganic
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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)
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

Solid-state lithium ion electrolytes of lithium potassium tantalate based compounds are provided which contain an anionic framework capable of conducting lithium ions. An activation energy of the lithium metal silicate composites is from 0.12 to 0.45 eV and conductivities are from 10−3 to 40 mS/cm at 300K. Compounds of specific formulae are provided and methods to alter the materials with inclusion of aliovalent ions shown. Lithium batteries containing the composite lithium ion electrolytes are also provided. Electrodes containing the lithium potassium tantalate based materials and batteries with such electrodes are also provided.

## Claims

### Claim 1

A solid-state lithium ion electrolyte, comprising:
at least one material selected from the group of materials consisting of compounds of formulae (I), (II), (III) and (IV):
Liy(M1)x1KTaO6 (I)
wherein x1 is a number from greater than 0 to less than 6, y is a value such that charge neutrality of the formula is obtained, and M1 is at least one element different from Li selected from elements of groups 1, 2, 13 and transition metals;
LiyK1-x2(M2)x2TaO6 (II)
wherein x2 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the composite formula is obtained, and M2 is at least one element different from K selected from elements of groups 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12 and 13;
LiyKTa1-x3(M3)x3O6 (III)
wherein x3 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the formula is obtained, and M3 is at least one element different from Ta selected from elements of groups 1-13; and
Li6KTaO6 (IV)

### Claim 2 (depends on 1)

The solid state lithium ion electrolyte according to claim 1, wherein
a lithium ion (Li+) conductivity of the solid state lithium ion electrolyte is from 10−3 to 40 mS/cm at 300K.

### Claim 3 (depends on 1)

The solid state lithium ion electrolyte according to claim 1, wherein
an activation energy of the material is from 0.12 to 0.45 eV.

### Claim 4 (depends on 1)

The solid state lithium ion electrolyte according to claim 1, wherein the material comprises a trigonal structure.

### Claim 5 (depends on 1)

The solid state lithium ion electrolyte according to claim 1 wherein an X-ray Diffraction Analysis obtained based on Cu-Kα radiation with wavelength of 1.54184 Å. of the material comprises the following major peaks:
Peak Position
Relative Intensity
17.50
100.00
21.61
97.58
27.73
61.36
27.94
41.39
35.42
21.89
37.89
24.22
41.87
67.06
43.61
13.99
44.03
18.73
47.73
17.13
52.83
15.17
54.30
19.38
57.73
10.11
57.85
11.10
59.46
13.37
61.94
19.62
62.38
11.77
68.43
10.53

### Claim 6

A solid state lithium battery, comprising:
an anode;
a cathode; and
a solid state lithium ion electrolyte located between the anode and the cathode;
wherein
the solid state lithium ion electrolyte comprises at least one material selected from the group of materials consisting compounds of formulae (I), (II), (III) and (IV):
Liy(M1)x1KTaO6 (I)
wherein x1 is a number from greater than 0 to less than 6, y is a value such that charge neutrality of the formula is obtained, and M1 is at least one element different from Li selected from elements of groups 1, 2, 13 and transition metals;
LiyK1-x2(M2)x2 TaO6 (II)
wherein x2 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the composite formula is obtained, and M2 is at least one element different from K selected from elements of groups 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12 and 13;
LiyKTa1-x3(M3)x3O6 (III)
wherein x3 is a number from greater than 0 to less than 1. y is a value such that charge neutrality of the formula is obtained, and M3 is at least one element different from Ta selected from elements of groups 1-13; and
Li6KTaO6 (IV)

### Claim 7 (depends on 6)

The solid state lithium ion battery according to claim 6, wherein the battery is a lithium metal battery or a lithium ion battery.

### Claim 8

An electrode for a solid state lithium battery, comprising:
a current collector; and
an electrode active layer on the current collector;
wherein the electrode active layer comprises at least one compound selected from the group consisting of compounds of formulae (I), (II), (III) and (IV):
Liy(M1)x1KTaO6 (I)
wherein x1 is a number from greater than 0 to less than 6, y is a value such that charge neutrality of the formula is obtained, and M1 is at least one element different from Li selected from elements of groups 1, 2, 13 and transition metals;
LiyK1-x2(M2)x2TaO6 (II)
wherein x2 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the composite formula is obtained, and M2 is at least one element different from K selected from elements of groups I, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12 and 13;
LiyKTa1-x3(M3)x3O6 (III)
wherein x3 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the formula is obtained, and M3 is at least one element different from Ta selected from elements of groups 1-13; and
Li6KTaO6 (IV)

### Claim 9

An electrode for a solid state lithium battery, comprising:
a current collector;
an electrode active layer on the current collector; and a coating layer on the electrode active layer;
wherein the coating layer on the electrode active layer comprises at least one compound selected from the group consisting of compounds of formulae (I), (II), (III) and (IV):
Liy(M1)x1KTaO6 (I)
wherein x1 is a number from greater than 0 to less than 6, y is a value such that charge neutrality of the formula is obtained, and M1 is at least one element different from Li selected from elements of groups 1, 2, 13 and transition metals;
LiyK1-x2(M2)x2TaO6 (II)
wherein x2 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the composite formula is obtained, and M2 is at least one element different from K selected from elements of groups 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12 and 13;
LiyKTa1-x3(M3)x3O6 (III)
wherein x3 is a number from greater than 0 to less than 1, y is a value such that charge neutrality of the formula is obtained, and M3 is at least one element different from Ta selected from elements of groups 1-13; and
Li6KTaO6 (IV)

### Claim 10 (depends on 8)

A solid state lithium battery comprising the electrode of claim 8, wherein the solid state lithium battery is a lithium ion battery or a lithium metal battery.

### Claim 11 (depends on 9)

A solid state lithium battery comprising the electrode of claim 9, wherein the solid state lithium battery is a lithium ion battery or a lithium metal battery.