# US 2018/0026302 A1 · High-performance ceramic-polymer separators for lithium batteries

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- Number: US 2018/0026302 A1
- Document ID: US20180026302A1
- Status: Published application
- Kind: A1
- Application number: 15/655,492
- Filed: 2017-07-20
- Published: 2018-01-25
- Earliest claimed: 2016-07-20
- Assignees: University of Dayton
- Applicants: University of Dayton
- Inventors: Jitendra Kumar; Guru Subramanyam
- Web page: https://patentgrep.com/patent/US20180026302A1

## CPC

- H01M 10/0565: Polymeric materials, e.g. gel-type or solid-type
- H01M 4/38: of elements or alloys
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- 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 10/052: Li-accumulators
- 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 10/0562: Solid materials
- H01M 50/403: Manufacturing processes of separators, membranes or diaphragms
- H01M 50/417: Polyolefins
- H01M 50/423: Polyamide resins
- H01M 50/434: Ceramics
- H01M 50/457: comprising three or more layers
- H01M 2300/0068: inorganic
- H01M 2300/0082: Organic polymers
- H01M 2300/0094: in the form of layered products, e.g. coatings
- Y02E 60/10: Energy storage using batteries
- Y02T 10/70: Energy storage systems for electromobility, e.g. 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
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION

## Abstract

An EB-PVD technique was used to fabricate ceramic/polymer/ceramic (LAGP/PE/LAGP) hybrid separator for rechargeable LIBs and Li batteries. The application of a ceramic electrolyte (LAGP) layer on traditional PE separator soaked in 1-M LiAsF6 liquid electrolyte combined the best attributes of traditional PE separator and solid inorganic electrolytes. The synergistic behavior of hybrid separator resulted in a high mechanical stability/flexibility, increased liquid uptake, high ion conduction, reduced cell voltage polarization, no lithium dendrite formation, and increased usable lithium content as compared to the state-of-the-art PE separator used in LIBs. The functional separator can be used to prolong life cycle and power capability of present LIBs. Thickness and density optimization of LAGP or similar electrolytes on polymer or other battery separators and their use in full Li battery (LIB, Li—S, Li—O2, Li-Ph, flow battery) cells are expected to further improve performance.

## Claims

### Claim 1

A lithium-ion battery comprising:
an anode;
a cathode; and
a hybrid electrolyte separator disposed between the anode and the cathode,
wherein:
the hybrid electrolyte separator comprises a polymer membrane, a first ceramic coating between the polymer membrane and the anode, and a second ceramic coating between the polymer membrane and the cathode.

### Claim 2 (depends on 1)

The lithium-ion battery of claim 1, wherein:
the polymer membrane is chosen from polyethylene, polyimides, or polyamides;
the first ceramic coating and the second ceramic coating are lithium-ion conductive materials independently chosen from lithium aluminum germanium phosphate (LAGP), lithium aluminum titanium phosphate (LATP), LiSICON, LiPON, perovskites, garnet-type ceramics, or phthalocyanines.

### Claim 3 (depends on 1)

The lithium-ion battery of claim 1, wherein:
the polymer membrane comprises polyethylene;
the first ceramic coating and the second ceramic coating comprise lithium aluminum germanium phosphate (LAGP).

### Claim 4 (depends on 3)

The lithium-ion battery of claim 3, wherein the first ceramic coating and the second ceramic coating are coated directly onto opposing surfaces of the polymer membrane.

### Claim 5 (depends on 3)

The lithium-ion battery of claim 3, wherein the LAGP has an empirical formula 19.75Li2O.6.17Al2O3.37.04GeO2.37.04P2O5.

### Claim 6 (depends on 3)

The lithium-ion battery of claim 3, wherein the anode, the cathode, and the hybrid electrolyte separator are disposed in a liquid electrolyte.

### Claim 7 (depends on 6)

The lithium-ion battery of claim 6, wherein the liquid electrolyte comprises LiPF6 in a solvent chosen from ethylene carbonate, dimethyl carbonate, ethylmethyl carbonate and mixtures thereof.

### Claim 8 (depends on 2)

The lithium-ion battery of claim 2, wherein the lithium-ion battery is configured as a Li-oxygen (Li—O2) cell, a Li-Phthalocyanine (Li-Ph) cell, a redox flow battery, a supercapacitor, or a hybrid battery-capacitor.

### Claim 9 (depends on 2)

The lithium-ion battery of claim 2, wherein the anode is lithium metal and the cathode is LiCoO2.

### Claim 10 (depends on 2)

The lithium-ion battery of claim 2, wherein the anode is lithium metal and the cathode comprises sulfur, LAGP, carbon nanotubes, and PVDF.

### Claim 11

A method for preparing a lithium battery, the method comprising:
depositing a first ceramic coating onto a first surface of a polymer membrane;
depositing a second ceramic coating onto a second surface of the polymer membrane opposite the first surface;
assembling the polymer membrane coated with the first ceramic coating and the second ceramic coating between an anode and a cathode such that the first ceramic coating faces the anode and the second ceramic coating faces the cathode, the anode comprising lithium metal.

### Claim 12 (depends on 11)

The method of claim 11, wherein both depositing the first ceramic coating and depositing the second ceramic coating comprise a coating process chosen from electron-beam physical vapor deposition, atomic layer deposition, sputtering, laser ablation, chemical vapor deposition, or combinations thereof.

### Claim 13 (depends on 11)

The method of claim 11, wherein both depositing the first ceramic coating and depositing the second ceramic coating comprise electron-beam physical vapor deposition.

### Claim 14 (depends on 11)

The method of claim 11, wherein:
the polymer membrane is chosen from polyethylene, polyimides, or polyamides;
the first ceramic coating and the second ceramic coating are lithium-ion conductive materials independently chosen from lithium aluminum germanium phosphate (LAGP), LiSICON, LiPON, lithium aluminum titanium phosphate (LATP), perovskites, garnet-type ceramics, or phthalocyanines.

### Claim 15 (depends on 11)

The method of claim 11, wherein:
the polymer membrane comprises polyethylene;
the first ceramic coating and the second ceramic coating comprise lithium aluminum germanium phosphate (LAGP).

### Claim 16 (depends on 11)

The method of claim 11, wherein the first ceramic coating and the second ceramic coating are deposited directly onto opposing surfaces of the polymer membrane.

### Claim 17 (depends on 11)

The method of claim 11, wherein the cathode is LiCoO2.

### Claim 18 (depends on 11)

The method of claim 11, wherein the cathode comprises sulfur, LAGP, carbon nanotubes, and PVDF.

### Claim 19

A hybrid electrolyte separator for a lithium-ion battery, the hybrid electrolyte separator comprising:
a polymer membrane;
a first ceramic coating on a first surface of the polymer membrane; and
a second ceramic coating on a second surface of the polymer membrane opposite the first surface,
wherein:
the polymer membrane is chosen from polyethylene, polyimides, or polyamides; and
the first ceramic coating and the second ceramic coating are lithium-ion conductive materials independently chosen from lithium aluminum germanium phosphate (LAGP), LiSICON, LiPON, perovskites, garnet-type ceramics, or phthalocyanines.

### Claim 20 (depends on 19)

The hybrid electrolyte separator or claim 19, wherein the polymer membrane is polyethylene and at least one of the first ceramic coating and the second ceramic coating is lithium aluminum germanium phosphate (LAGP).