# US 2021/0344036 A1 · Nanostructured lithium-ion battery electrode composite materials via conformal graphene dispersion

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- Number: US 2021/0344036 A1
- Document ID: US20210344036A1
- Status: Published application
- Kind: A1
- Application number: 17/369,058
- Filed: 2021-07-07
- Published: 2021-11-04
- Earliest claimed: 2017-02-27
- Assignees: Northwestern University
- Applicants: Northwestern University
- Inventors: Mark C. Hersam; Kan-Sheng Chen; Ethan B. Secor
- Web page: https://patentgrep.com/patent/US20210344036A1

## CPC

- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 4/0416: {involving impregnation with a solution, dispersion, paste or dry powder (H01M4/0438 takes precedence)}
- H01M 4/131: Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/133: Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/136: Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
- H01M 4/139: Processes of manufacture
- H01M 4/1393: of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/505: of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
- H01M 4/625: {Carbon or graphite}
- H01M 2004/027: {Negative electrodes}
- H01M 2004/028: {Positive electrodes}
- 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

Composites comprising anode and cathode active materials conformally coupled to few-layered graphene, corresponding electrodes and related methods of preparation.

## Claims

### Claim at position 1

1-33. (canceled)

### Claim 34

A method of using a graphene-cellulosic polymer composition to modulate lithium-ion battery cathode performance, said method comprising:
contacting an exfoliated graphene-cellulosic polymer composition with a composition comprising nanoparticulate LMO and a hydrophobic fluid component;
depositing said compositions on a lithium-ion battery cathode substrate; and
annealing said deposited compositions to conformally coat a said LMO nanoparticle with at least one of said graphene and an annealation product of said cellulosic polymer, thereby modulating at least one of the packing density of said LMO nanoparticles and manganese ion dissolution from said nanoparticles.

### Claim 35 (depends on 34)

The method of claim 34 wherein said cellulosic polymer is an ethyl cellulose.

### Claim 36 (depends on 34)

The method of claim 34 wherein said hydrophobic fluid component is selected from C2-C5 alcohols, esters, amides, ethers and ketones and combinations thereof.

### Claim 37 (depends on 36)

The method of claim 36 wherein said hydrophobic fluid component comprises N-methyl-2-pyrrolidone.

### Claim 38 (depends on 34)

The cathode of claim 34 wherein the packing density of said LMO is greater than about 2.0 g cm−3.

### Claim 39 (depends on 34)

The cathode of claim 34 wherein said LMO is at least about 80 wt. % of said composite.

### Claim 40 (depends on 34)

The method of claim 34 comprising incorporation of said cathode into a lithium-ion battery, thereby reducing manganese ion dissolution into the electrolyte of said battery.

### Claim 41

A method for forming a composite, comprising:
agitating a mixture of nanoparticles of a material selected from lithium-ion cathode active materials for a lithium-ion battery and lithium-ion anode active materials for a lithium-ion battery, few-layered graphene comprising mono-, bi- and n-layered graphene, n being an integer selected from 3 to 6, and ethyl cellulose in a solvent to disperse said nanoparticles and said few-layered graphene with the ethyl cellulose so as to prevent aggregation of said nanoparticles;
evaporating the solvent from the mixture to form a dispersion of said nanoparticles and said few-layered graphene with the ethyl cellulose; and
ambient annealing the dispersion at a temperature for a period of time to decompose the ethyl cellulose, thereby resulting in said composite,
wherein in said composite, said nanoparticles are evenly mixed with said few-layered graphene, and individual said nanoparticles, rather than multi-particle particulates, are conformally coated with a combination of said few-layered graphene and said annealation product of the ethyl cellulose that comprises amorphous carbon with sp2-carbon content, such that Raman spectroscopy of said composite has a peak at 2D-band; and
wherein said few-layered graphene is not graphene oxide and is not reduced graphene oxide.

### Claim 42 (depends on 41)

The method of claim 41, wherein said cathode active material is selected from lithium cobalt oxide, lithium iron phosphate, lithium manganese oxide (LMO), lithium nickel manganese cobalt oxide and lithium nickel cobalt aluminum oxide.

### Claim 43 (depends on 42)

The method of claim 42, wherein said active material is LMO.

### Claim 44 (depends on 43)

The method of claim 43, wherein said nanoparticles comprise a spinel LMO structure.

### Claim 45 (depends on 41)

The method of claim 41, wherein said anode active material is selected from lithium titanate, natural graphite, artificial graphite, activated carbon, carbon black and silicon.

### Claim 46 (depends on 41)

The method of claim 41, wherein the temperature is 285° C., and the period of time is 3 hours.