# US 2021/0280853 A1 · All-solid secondary battery and method of preparing the same

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- Number: US 2021/0280853 A1
- Document ID: US20210280853A1
- Status: Published application
- Kind: A1
- Application number: 17/093,989
- Filed: 2020-11-10
- Published: 2021-09-09
- Earliest claimed: 2020-03-09
- Assignees: Samsung Electronics Co., Ltd.
- Applicants: Samsung Electronics Co., Ltd.
- Inventors: Sewon KIM; Sungkyun JUNG; Naoki SUZUKI; Satoshi FUJIKI; Tomoyuki TSUJIMURA; Hyeokjo GWON; Jusik KIM
- Web page: https://patentgrep.com/patent/US20210280853A1

## CPC

- H01M 4/366: {as layered products}
- H01M 4/0407: {by coating on an electrolyte layer}
- H01M 4/043: {involving compressing or compaction}
- 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 4/1393: of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/1395: of electrodes based on metals, Si or alloys
- H01M 4/382: {Lithium (H01M4/405 takes precedence)}
- H01M 4/405: {Alloys based on lithium}
- H01M 4/587: for inserting or intercalating light metals
- H01M 10/052: Li-accumulators
- 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 10/4235: {Safety or regulating additives or arrangements in electrodes, separators or electrolyte (H01M10/4242 takes precedence)}
- H01M 2004/027: {Negative electrodes}
- H01M 2300/0071: Oxides
- 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

An all-solid secondary battery, including: a cathode; an anode; and a solid electrolyte layer disposed between the cathode and the anode, wherein the anode comprises an anode current collector; a first anode active material layer in contact with the anode current collector and comprising a first metal; a second anode active material layer disposed between the first anode active material layer and the solid electrolyte layer and comprising a carbon-containing active material; and a contact layer between the second anode active material layer and the solid electrolyte layer, and disposed such that the contact layer prevents contact between the second anode active material layer and the solid electrolyte layer, wherein the contact layer comprises a second metal, and has a thickness less than a thickness of the first anode active material layer.

## Claims

### Claim 1

An all-solid secondary battery, comprising:
a cathode;
an anode; and
a solid electrolyte layer disposed between the cathode and the anode,
wherein the anode comprises
an anode current collector;
a first anode active material layer in contact with the anode current collector and comprising a first metal;
a second anode active material layer disposed between the first anode active material layer and the solid electrolyte layer and comprising a carbon-containing active material; and
a contact layer between the second anode active material layer and the solid electrolyte layer, and disposed such that the contact layer prevents contact between the second anode active material layer and the solid electrolyte layer,
wherein the contact layer comprises a second metal, and has a thickness less than a thickness of the first anode active material layer.

### Claim 2 (depends on 1)

The all-solid secondary battery of claim 1, wherein the first metal comprises lithium metal or a lithium alloy, and the second metal comprises lithium metal or a lithium alloy.

### Claim 3 (depends on 2)

The all-solid secondary battery of claim 2, wherein the first metal and the second metal are the same.

### Claim 4 (depends on 1)

The all-solid secondary battery of claim 1, wherein the thickness of the contact layer is 20% or less of the thickness of the first anode active material layer.

### Claim 5 (depends on 1)

The all-solid secondary battery of claim 1, wherein the thickness of the contact layer is about 1 nanometer to about 1 micrometer.

### Claim 6 (depends on 1)

The all-solid secondary battery of claim 1, wherein the thickness of the contact layer is less than a thickness of the second anode active material layer.

### Claim 7 (depends on 1)

The all-solid secondary battery of claim 1, wherein the contact layer does not comprise a carbon-containing material.

### Claim 8 (depends on 1)

The all-solid secondary battery of claim 1, wherein during a charge/discharge cycle, a volume change rate of the first anode active material layer is greater than a volume change rate of the contact layer.

### Claim 9 (depends on 1)

The all-solid secondary battery of claim 1, wherein during a charge/discharge cycle, a volume change rate of the second anode active material layer is greater than a volume change rate of the contact layer

### Claim 10 (depends on 1)

The all-solid secondary battery of claim 1, wherein a volume of the contact layer after charge is about 1.5 times to about 20 times a volume of the contact layer after discharge.

### Claim 11 (depends on 1)

The all-solid secondary battery of claim 1, wherein a volume of the first anode active material layer after charge is about 1.5 times to about 500 times a volume of the first anode active material layer after discharge.

### Claim 12 (depends on 1)

The all-solid secondary battery of claim 1, wherein a volume of the second anode active material layer after charge is greater than a volume of the second anode active material layer after discharge, and the volume of the second anode active material layer after charge is about 2 times or less the volume of second anode active material layer after discharge.

### Claim 13 (depends on 1)

The all-solid secondary battery of claim 1, wherein the solid electrolyte layer comprises an oxide-containing solid electrolyte.

### Claim 14

A method of preparing an all-solid secondary battery, the method comprising:
providing a cathode layer;
providing an anode layer;
providing a solid electrolyte layer;
attaching the anode layer to a surface of the solid electrolyte layer; and
attaching the cathode layer to another surface of the solid electrolyte layer, wherein the providing of the anode layer comprises:
disposing a first layer comprising lithium metal or a lithium alloy on a first substrate,
disposing a second layer comprising a carbon-containing active material on a second substrate,
disposing the first layer and the second layer to face each other, and pressing the first substrate and the second substrate such that the first substrate and the second substrate move closer to each other,
wherein in the process of pressing the first substrate and the second substrate, a third layer comprising lithium metal or a lithium alloy is formed between the second substrate and the second layer, and the third layer has a thickness less than a thickness of the first layer.

### Claim 15 (depends on 14)

The method of claim 14, wherein
the second layer comprises a metal alloyable with lithium, and
in the pressing of the first substrate and the second substrate, the metal alloyable with lithium forms an alloy with lithium in the first layer and in the third layer.

### Claim 16 (depends on 14)

The method of claim 14, wherein in the providing of the anode layer further comprises, removing the second substrate after the third layer is formed.

### Claim 17 (depends on 14)

The method of claim 14, wherein a pressure applied in the pressing of the first substrate and the second substrate is about 150 megapascals to about 1,000 megapascals.

### Claim 18

A method of preparing an anode layer of an all-solid secondary battery, the method comprising:
providing a first layer comprising lithium metal or a lithium alloy disposed on a first substrate,
providing a second layer comprising a carbon-based active material disposed on a second substrate;
disposing the first layer and the second layer to face each other; and
pressing the first substrate and the second substrate such that the first substrate and the second substrate are move closer to each other,
wherein, in the pressing of the first substrate and the second substrate,
a third layer comprising lithium metal or a lithium alloy is formed between the second substrate and the second layer, and the third layer has a thickness less than a thickness of the first layer.

### Claim 19 (depends on 18)

The method of claim 18, wherein
the second layer comprises a metal alloyable with lithium, and
in the pressing of the first substrate and the second substrate, the metal alloyable with lithium forms an alloy with lithium in the first layer and in the third layer, a pressure applied in the pressing of the first substrate and the second substrate is about 150 megapascals to about 1,000 megapascals.

### Claim 20 (depends on 18)

The method of claim 18, wherein the providing of the anode layer further comprises removing the second substrate after the third layer is formed.