# US 2019/0355992 A1 · Cathode stabilization method using electrochemical oxidative additives in aqueous alkali-ion batteries

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- Number: US 2019/0355992 A1
- Document ID: US20190355992A1
- Status: Published application
- Kind: A1
- Application number: 16/471,886
- Filed: 2017-12-20
- Published: 2019-11-21
- Earliest claimed: 2016-12-20
- Assignees: University of Maryland, College Park
- Applicants: University of Maryland, College Park
- Inventors: Chunsheng WANG; Fei WANG
- Web page: https://patentgrep.com/patent/US20190355992A1

## CPC

- H01M 4/628: {Inhibitors, e.g. gassing inhibitors, corrosion inhibitors}
- H01M 4/0445: {Forming after manufacture of the electrode, e.g. first charge, cycling}
- H01M 4/366: {as layered products}
- H01M 4/505: of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
- H01M 4/525: of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
- H01M 4/5825: {Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 10/056: characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M 10/0567: characterised by the additives
- H01M 10/36: Accumulators not provided for in groups H01M10/05-H01M10/34
- H01M 2004/028: {Positive electrodes}
- H01M 2300/0002: Aqueous electrolytes
- H01M 2300/0088: Composites
- Y02E 60/10: Energy storage using batteries
- 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

## Abstract

The present invention is directed to aqueous solid state electrolytes that comprises an oxidative additive to stabilize the interface between the cathode and aqueous electrolyte. The present invention is also directed to methods of making the solid state electrolyte materials and methods of using the solid state electrolyte materials in batteries and other electrochemical technologies.

## Claims

### Claim 1

A cathode comprising:
(a) a cathode active material; and
(b) a solid electrolyte interphase layer;
wherein the solid electrolyte interface layer covers the cathode active material.

### Claim 2 (depends on 1)

The cathode of claim 1, wherein the cathode active material is a lithium metal oxide or a lithium metal phosphate.

### Claim at position 3

-4. (canceled).

### Claim 5 (depends on 1)

The cathode of claim 1, wherein the cathode active material is selected from the group consisting of LiFePO4, LiMn2O4, LiCoO2, LiNi0.33Mn0.33Co0.33O2, LiNi0.6Mn0.2Co0.2O2, LiNi0.8Mn0.1Co0.1O2, LiNi0.5Mn1.5O4, LiNi0.8Co0.15Al0.05O2, and LiMnPO4.

### Claim 6

(canceled)

### Claim 7 (depends on 1)

The cathode of claim 1, wherein the solid electrolyte interphase layer is a decomposition product of at least one oxidative additive.

### Claim at position 7

-10. (canceled)

### Claim 11 (depends on 1)

The cathode of claim 1, wherein the solid electrolyte interphase layers covers between about 40% and about 100% of the cathode active material.

### Claim 12

An electrochemical cell comprising:
(a) an anode;
(b) a cathode; and
(c) an aqueous or a hybrid electrolyte;
wherein the cathode comprises a solid electrolyte interphase layer that covers a cathode active material.

### Claim 13 (depends on 12)

The electrochemical cell of claim 12, wherein the cathode active material is a lithium metal oxide or a lithium metal phosphate.

### Claim at position 11

-15. (canceled)

### Claim 16 (depends on 12)

The electrochemical cell of claim 12, wherein the cathode active material is selected from the group consisting of LiFePO4, LiMn2O4, LiCoO2, LiNi0.33Mn0.33Co0.33O2, LiNi0.6Mn0.2Co0.2O2, LiNi0.8Mn0.1Co0.1O2, LiNi0.5Mn1.5O4, LiNi0.8Co0.15Al0.05O2, and LiMnPO4

### Claim 17

(canceled)

### Claim 18 (depends on 12)

The electrochemical cell of any one of claim 12, wherein the solid electrolyte interphase layer is a decomposition product of at least one oxidative additive.

### Claim at position 15

-22. (canceled)

### Claim 23 (depends on 12)

The electrochemical cell of claim 12, wherein the solid electrolyte interphase layers covers between about 40% and about 100% of the cathode active material.

### Claim 24

(canceled)

### Claim 25 (depends on 12)

The electrochemical cell of claim 12, wherein the aqueous or hybrid electrolyte is selected from the group consisting of LiN(SO2CF3)2, LiN(SO2CH3)2, LiN(SO2C4H9)2, LiN(SO2C2F5)2, LiN(SO2C4F9)2, LiN(SO2F3)(SO2C4F9), LiN(SO2C2F5)(SO2C4F9), LiN(SO2C2F4SO2), LiN(SO2F)2, and LiN(SO2F)(SO2CF3).

### Claim 26

(canceled)

### Claim 27 (depends on 12)

The electrochemical cell of claim 12, wherein the anode is selected from the group consisting of lithium, magnesium, aluminum, molybdenum, zinc, chromium, iron, nickel, tin, lead, copper, silver, palladium, mercury, platinum, gold, combinations thereof, metal alloys thereof, metal oxides thereof, metal phosphates thereof, and metal sulfides thereof.

### Claim at position 21

-29. (canceled)

### Claim 30 (depends on 12)

The electrochemical cell of claim 12, wherein the capacity decay rate (mAh/g) at a C-rate of about 2.5 C is between about 0.005% and about 0.1% per cycle.

### Claim 31

(canceled)

### Claim 32 (depends on 12)

The electrochemical cell of claim 12, wherein the energy density at a C-rate of about 0.5 C is between about 20 Wh/kg and about 200 Wh/kg.

### Claim 33

(canceled)

### Claim 34

A process for preparing a cathode for an electrochemical device comprising:
(a) providing a cathode active material;
(b) immersing the cathode active material in an aqueous or hybrid electrolyte comprising at least one oxidative additive; and
(c) charging the cathode active material to form a solid electrolyte material upon the cathode active material.

### Claim 35 (depends on 34)

The process of claim 34, wherein the cathode active material is a lithium metal oxide or a lithium metal phosphate.

### Claim at position 28

-37. (canceled)

### Claim 38 (depends on 34)

The process of claim 34, wherein the cathode active material is selected from the group consisting of LiFePO4, LiMn2O4, LiCoO2, LiNi0.33Mn0.33Co0.33O2, LiNi0.6Mn0.2Co0.2O2, LiNi0.8Mn0.1Co0.1O2, LiNi0.5Mn1.5O4, LiNi0.8Co0.15Al0.05O2, and LiMnPO4.

### Claim at position 30

-40. (canceled)

### Claim 41 (depends on 34)

The process of claim 34, wherein the at least one oxidative additive is selected from the group consisting of biphenyl, aniline, 2,2-diphenylpropane, t-butylbenzene, cyclohexylbenzene, thiophene, 3-chlorothiophene, 3-hexylthiophene, furan, furfural, benzofuran, pyrrole, indole, tris(trimethylsilyl)phosphate, tris(hexafluoroisopropyl)phosphate, triallyl phosphate, N,N-diethylamino trimethyl silane, tris(pentafluorophenyl)silane, phenyl tris-2-methoxydiethoxy silane, tris(trimethylsilypborate, lithium bis(oxalate)borate, trimethyl borate, and triethyl borate,

### Claim 42

(canceled)

### Claim 43 (depends on 34)

The process of claim 34, wherein the solid electrolyte interphase layer covers between about 40% and about 100% of the cathode active material.

### Claim 44 (depends on 34)

The process of claim 34, comprising between about 0.05% and about 20% mass percentage of the at least one oxidative additive, wherein the mass percentage is measured by total mass of the oxidative additive and the aqueous or hybrid electrolyte.