Lithium Metal-Glass Electrolyte Lamination for Low-Resistance Interfaces

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Solution Overview

Problem

Lithium metal foils in all-solid-state secondary batteries face challenges with native oxide films that affect layer adhesion and interfacial resistance when laminated with solid electrolyte layers, leading to performance issues and potential delamination.

Innovation Solution

A high homologous temperature lamination process is used to absorb the native oxide film of lithium-containing metal foils with a sulfide glass electrolyte layer, forming a laminating layer that enhances adhesive strength and reduces interfacial resistance, allowing for a robust and pressure-independent laminate.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Device complexity

If lithium metal foil is directly laminated to solid electrolyte layer, then battery assembly is simple, but layer adhesion is poor due to native oxide film

Engineering Contradiction:
Improvebattery assembly processVSAvoidlayer adhesion
Core Design Contradiction:
Device complexityVSStrength

Solution Approach 1:

The patent applies preliminary action by forming a native oxide film on the lithium metal surface before lamination, then utilizing high homologous temperature processing to transform this pre-formed oxide into a beneficial interfacial layer that enhances adhesion between the lithium metal and solid electrolyte

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent changes the temperature parameter to high homologous temperature (close to the melting point of lithium) during lamination, which transforms the native oxide film from a harmful barrier into a reactive intermediate that improves interfacial bonding and reduces contact resistance

Inventive Principle:
Principle #35Parameter changes

2Strength

If native oxide film is removed from lithium metal surface, then layer adhesion improves, but interfacial resistance increases

Engineering Contradiction:
Improvelayer adhesionVSAvoidinterfacial resistance
Core Design Contradiction:
StrengthVSReliability

Solution Approach 1:

The patent converts the harmful native oxide film into a beneficial interfacial layer by processing at high homologous temperature, where the oxide reacts with the solid electrolyte to form a low-resistance interface that simultaneously provides good adhesion and electrical conductivity

Inventive Principle:
Principle #22Blessing in disguise (Convert harm into benefit)

3Use of energy by moving object

If lamination is performed at room temperature, then energy consumption is low, but adhesive strength is insufficient

Engineering Contradiction:
Improveenergy consumptionVSAvoidadhesive strength
Core Design Contradiction:
Use of energy by moving objectVSStrength

Solution Approach 1:

The patent utilizes phase transition by heating the lithium metal to high homologous temperature, approaching its melting point, which increases atomic mobility and enables diffusion bonding between the lithium metal and solid electrolyte, creating strong adhesion that persists at room temperature

Inventive Principle:
Principle #36Phase transitions

4Reliability

If high homologous temperature lamination is used, then adhesive strength and conductivity improve, but processing complexity increases

Engineering Contradiction:
Improveadhesive strength and conductivityVSAvoidprocessing complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The patent merges the lamination and heat treatment steps into a single high homologous temperature processing step, where pressing and heating occur simultaneously to form the bonded interface, reducing the number of separate processing operations

Inventive Principle:
Principle #5Merging (Combining)

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 process results in a negative electrode-glass electrolyte laminate with significantly reduced interfacial resistance and improved adhesion, enabling efficient lithium ion conductivity and stable battery performance without the need for additional pressing, thus enhancing energy density and safety.

Implementation Method 1

the lamination is performed in a manner and at sufficiently high homologous temperature of the metal foil such that any native film (e.g., oxide, carbonate or combination thereof) on the surface of the foil is absorbed by what is termed herein a 'laminating layer' which reactively forms at the interface

Methodology Applied
Scientific EffectAbsorption: Absorption (physical)

Implementation Method 2

a laminating layer which reactively forms at the interface

Methodology Applied
Scientific EffectChemical bonding: Chemical Bonding

Implementation Method 3

it expresses the temperature of a material as a fraction of its melting point temperature, using the Kelvin scale. Accordingly, this allows for comparison of the working conditions of different lithium-containing metal foils and is therefore relatable to diffusion dependent deformation which may take place when laminating at high temperatures

Methodology Applied
Scientific EffectDiffusion: Diffusion

Data Source

PatentUS20240039037A1Negative electrode-glass electrolyte layer laminate, all-solid-state secondary battery including the same, and method of manufacturing the same
Publication Date: 2024.02.01 SK ON CO LTD
  • US20240039037A1 patent drawing
  • US20240039037A1 patent drawing
  • US20240039037A1 patent drawing

AI summary

A negative electrode-glass electrolyte layer laminate including a negative electrode and a glass electrolyte layer on at least one surface of the negative electrode, wherein the negative electrode includes a surface passivated lithium-containing metal foil, and the laminate electrochemically operable in the absence of external pressure, an all-solid-state secondary battery including the negative electrode-glass electrolyte layer laminate, and a method of manufacturing the negative electrode-glass electrolyte layer laminate.