Lithium potassium tantalate compounds as Li super-ionic conductor, solid electrolyte and coating layer for lithium metal battery and lithium-ion battery

Patent metadata

Field	Value
Publication number	US-11145896-B2
Application number	US-201916570811-A
Country	US
Kind code	B2
Filing date	Sep 13, 2019
Priority date	Sep 13, 2019
Publication date	Oct 12, 2021
Grant date	Oct 12, 2021

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.

First claim

The invention claimed is:

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):
Li y (M1) x1 KTaO 6   (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;
Li y K 1-x2 (M2) x2 TaO 6   (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;
Li y KTa 1-x3 (M3) x3 O 6   (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
Li 6 KTaO 6   (IV)

2. 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.

3. 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.

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

5. 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.

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):
Li y (M1) x1 KTaO 6   (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;
Li y K 1-x2 (M2) x2 TaO 6   (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;
Li y KTa 1-x3 (M 3 ) x3 O 6   (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
Li 6 KTaO 6   (IV)

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

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):
Li y (M1) x1 KTaO 6   (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;
Li y K 1-x2 (M2) x2 TaO 6   (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;
Li y KTa 1-x3 (M3) x3 O 6   (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
Li 6 KTaO 6   (IV)

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):
Li y (M1) x1 KTaO 6   (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;
Li y K 1-x2 (M2) x2 TaO 6   (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 eleme

Assignees

• Univ Maryland
• Toyota Eng & Mfg North America

Inventors

• Mo Yifei
• Bai Qiang
• He Xingfeng
• Ling Chen

Classifications

• H01M2004/027

  Negative electrodes · CPC title

• H01M10/052

  Li-accumulators · CPC title

• Y02E60/10

  Energy storage using batteries · CPC title

• H01M4/382

  Lithium (H01M4/405 takes precedence) · CPC title

• H01M10/0525 Primary

  Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries · CPC title