All-Solid Battery Interlayer Reduces Resistance

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Solution Overview

Problem

All-solid secondary batteries face challenges with interfacial resistance and lifespan deterioration due to lithium metal deposition and side reactions with the solid electrolyte, leading to potential short circuits and reduced safety.

Innovation Solution

A negative electrode-solid electrolyte sub-assembly is introduced, featuring a carbonaceous negative active material layer with an interlayer composed of a composite including a metal material and lithium ion conductor, which reduces interfacial resistance and buffers volume expansion, preventing cracking and improving cycle characteristics.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If lithium metal is used as negative active material to increase energy density, then capacity density is improved (about 10 times that of graphite), but interfacial resistance increases and lifespan deteriorates due to side reactions with solid electrolyte

Engineering Contradiction:
Improvecapacity densityVSAvoidlifespan
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

A buffer layer comprising a metal element (such as Al, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, Ge, In, Sn, Sb, or their alloys) is introduced between the lithium metal negative active material and the solid electrolyte. This intermediary buffer layer prevents direct contact and side reactions between lithium metal and the solid electrolyte, thereby reducing interfacial resistance and improving lifespan while maintaining the high capacity density of lithium metal.

Inventive Principle:
Principle #24Intermediary (Mediator)

2Use of energy by moving object

If lithium metal is used as negative active material, then energy density is improved, but short circuit risk increases due to lithium metal deposition and side reactions

Engineering Contradiction:
Improveenergy densityVSAvoidshort circuit risk
Core Design Contradiction:
Use of energy by moving objectVSObject-affected harmful factors

Solution Approach 1:

The buffer layer acts as a protective intermediary between lithium metal and the solid electrolyte, preventing harmful side reactions and lithium metal deposition that could lead to short circuits. This allows the system to maintain high energy density from lithium metal while eliminating the associated safety risks.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Reliability

If carbonaceous negative active material is used, then safety is improved by avoiding flammable organic solvents, but capacity density is reduced (about 1/10 that of lithium metal)

Engineering Contradiction:
ImprovesafetyVSAvoidcapacity density
Core Design Contradiction:
ReliabilityVSQuantity of substance

Solution Approach 1:

The invention merges the safety advantages of carbonaceous materials (or absence of flammable organic solvents) with the high capacity density of lithium metal. By using lithium metal as the negative active material in an all-solid battery configuration without flammable organic solvents, and adding a protective buffer layer, the system achieves both high safety and high capacity density simultaneously.

Inventive Principle:
Principle #5Merging (Combining)

4Reliability

If interlayer with metal material and lithium ion conductor is introduced, then interfacial resistance is reduced and cycle stability is enhanced, but device complexity increases

Engineering Contradiction:
Improvecycle stabilityVSAvoidstructure complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The buffer layer serves as a simple yet effective intermediary structure between the negative active material and solid electrolyte. While it does add a layer to the structure, the buffer layer can be formed by straightforward methods such as sputtering, evaporation, or chemical deposition, and uses common metal elements, thus minimizing the increase in device complexity while delivering significant improvements in interfacial resistance and cycle stability.

Inventive Principle:
Principle #24Intermediary (Mediator)

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

The solution effectively reduces interfacial resistance, enhances cycle stability, and prevents short circuits, thereby improving the safety and performance of all-solid secondary batteries.

Implementation Method 1

an interlayer on the first negative active material layer; and a solid electrolyte on the interlayer and opposite the first negative active material layer, wherein the interlayer includes a composite including a first metal material and a lithium ion conductor

Methodology Applied
Scientific EffectIon conduction: Fast Ion Conductor

Implementation Method 2

the interlayer includes a composite including a first metal material and a lithium ion conductor... buffers volume expansion, preventing cracking

Methodology Applied
Scientific EffectVolume expansion buffering: Elasticity

Data Source

PatentEP4184604A1Negative electrode for all-solid secondary battery, all-solid secondary battery including negative electrode, and method of preparing all-solid secondary battery
Publication Date: 2023.05.24 SAMSUNG ELECTRONICS CO LTD
  • EP4184604A1 patent drawingFigure 1A
  • EP4184604A1 patent drawingFigure 1B
  • EP4184604A1 patent drawingFigure 2A

AI summary

A negative electrode-solid electrolyte sub-assembly for an all-solid secondary battery, the sub-assembly including: a negative electrode current collector; a first negative active material layer on the current collector; an interlayer on the first negative active material layer; and a solid electrolyte on the interlayer and opposite the first negative active material layer, wherein the interlayer includes a composite including a first metal material and a lithium ion conductor, wherein the first metal material includes a first metal, an alloy including the first metal and lithium, a compound including the first metal and lithium, or a combination thereof, wherein the first negative active material layer includes a carbonaceous negative active material, and optionally a first negative active material including a second metal, a metalloid, or a combination thereof.