# US 2021/0280908 A1 · Composite electrolyte membrane and all-solid-state battery comprising the composite electrolyte membrane

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- Number: US 2021/0280908 A1
- Document ID: US20210280908A1
- Status: Published application
- Kind: A1
- Application number: 17/260,058
- Filed: 2019-10-10
- Published: 2021-09-09
- Earliest claimed: 2018-10-11
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Ji-Hoon RYU; Eun-Bee KIM; Suk-Woo LEE; Jung-Pil LEE
- Web page: https://patentgrep.com/patent/US20210280908A1

## CPC

- H01M 10/0565: Polymeric materials, e.g. gel-type or solid-type
- H01M 50/403: Manufacturing processes of separators, membranes or diaphragms
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 10/0562: Solid materials
- H01M 10/0585: of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
- H01M 50/417: Polyolefins
- H01M 50/449: having a layered structure
- H01M 50/489: Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
- H01M 2300/0082: Organic polymers
- H01M 2300/0094: in the form of layered products, e.g. coatings
- Y02E 60/10: Energy storage using batteries
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- 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
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

A composite electrolyte membrane according to the present disclosure includes a phase change layer on a surface in contact with an electrode, for example, a positive electrode. The phase change layer includes a filler, and a physically isolated area between the positive electrode and the composite electrolyte membrane, known as a dead space, is filled with the filler that is liquefied by heat resulting from the increased internal temperature of the battery, thereby reducing the interfacial resistance between the electrolyte membrane and the electrode.

## Claims

### Claim 1

A composite electrolyte membrane for an all-solid-state battery, comprising:
an electrolyte layer and a phase change layer stacked in a sequential order,
wherein the phase change layer comprises a porous sheet including a plurality of pores, and a filler with which the pores of the porous sheet are filled,
wherein the porous sheet includes a first polymer resin, and the filler exists in a solid state at 26° C. or less and a liquid state at 35° C. or above.

### Claim 2 (depends on 1)

The composite electrolyte membrane for an all-solid-state battery according to claim 1, wherein the filler comprises at least one selected from the group consisting of ethylene carbonate (EC), polyethylene glycol (PEG) having a weight average molecular weight of 1,000 or above, succinonitrile (SN), and cyclic phosphate (CP).

### Claim 3 (depends on 1)

The composite electrolyte membrane for an all-solid-state battery according to claim 1, wherein the electrolyte layer comprises at least one selected from the group consisting of a sulfide-based solid electrolyte, an oxide-based solid electrolyte and a polymer-based solid electrolyte, and wherein the polymer-based solid electrolyte comprises a second polymer resin and a lithium salt.

### Claim 4 (depends on 3)

The composite electrolyte membrane for an all-solid-state battery according to claim 3, wherein the electrolyte layer comprises the polymer-based solid electrolyte, and further wherein a layer comprising the second polymer resin and the lithium salt are coated on all or at least part of a surface of the polymer-based solid electrolyte that is in contact with the phase change layer.

### Claim 5 (depends on 3)

The composite electrolyte membrane for an all-solid-state battery according to claim 3, wherein the electrolyte layer comprises the polymer-based solid electrolyte, wherein the second polymer resin comprises at least one selected from the group consisting of polyether-based polymer, polycarbonate-based polymer, acrylate-based polymer, polysiloxane-based polymer, phosphagen-based polymer, a polyethylene derivative, an alkylene oxide derivative, phosphoric acid ester polymer, poly agitation lysine, polyester sulfide, polyvinyl alcohol, and polyvinylidene fluoride, and wherein the lithium salt and the polymer resin are mixed at a mole ratio of 1:5 to 1:30.

### Claim 6 (depends on 1)

The composite electrolyte membrane for an all-solid-state battery according to claim 1, wherein the porous sheet is a film or a non-woven fabric, wherein the non-woven fabric comprises a polyolefin-based polymer resin, and wherein the film or non-woven fabric has a porosity of 30 vol % to 80 vol %.

### Claim 7 (depends on 1)

An all-solid-state battery, comprising:
a negative electrode,
a positive electrode and
a composite electrolyte membrane according to claim 1;
wherein the composite electrolyte membrane is interposed between the negative electrode and the positive electrode, and
wherein the electrolyte layer of the composite electrolyte membrane is disposed in contact with the negative electrode, and the phase change layer is disposed in contact with the positive electrode.

### Claim 8 (depends on 7)

The all-solid-state battery according to claim 7, wherein the filler in the phase change layer is liquefied and kept in the liquefied state by reaction with the lithium salt, and the liquefied filler material is maintained to be filled in interfaces between the phase change layer and the electrolyte layer and between the phase change layer and the positive electrode.

### Claim 9

A method for manufacturing an all-solid-state battery, comprising:
(S1) preparing a negative electrode;
(S2) forming a solid electrolyte layer on a surface of the negative electrode;
(S3) preparing a porous sheet and filling the porous sheet with a liquid filler;
(S4) cooling a result of (S3) to solidify the liquid filler to form a phase change layer;
(S5) stacking the phase change layer on the electrolyte layer; and
(S6) preparing a positive electrode and stacking the positive electrode on the phase change layer.

### Claim 10 (depends on 9)

The method for manufacturing an all-solid-state battery according to claim 9, further comprising:
before the step (S5),
(S7) coating a lithium salt on the electrolyte layer to form a lithium salt layer.

### Claim 11 (depends on 9)

The method for manufacturing an all-solid-state battery according to claim 9, further comprising:
(S8) heating the battery manufactured after the step (S6) and leaving the battery for a predetermined time to liquefy the filler.
