Sulfide Solid Electrolyte Crystallinity Without Lithium Instability

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Solution Overview

Problem

Conventional crystalline sulfide-based solid electrolytes require high-temperature heat treatment to achieve high crystallinity, leading to instability with lithium metal and increased electronic conductivity, which can cause side reactions and short circuits in all-solid-state batteries.

Innovation Solution

A Li2S—P2S5-MCl-MX′ (X′ being a halogen other than Cl) sulfide-based solid electrolyte with a specific molar ratio of elements, heat-treated at 450° C. to 500° C. under vacuum or inert atmosphere, minimizing sulfur vacancy and electronic conductivity while maintaining high ionic conductivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Stability of the object's composition

If heat treatment temperature is increased to achieve high crystallinity, then crystallinity is improved, but stability with lithium metal deteriorates and electronic conductivity increases

Engineering Contradiction:
ImprovecrystallinityVSAvoidstability with lithium metal
Core Design Contradiction:
Stability of the object's compositionVSReliability

Solution Approach 1:

The patent optimizes the heat treatment temperature parameter to a specific range (400-500°C) that achieves high crystallinity while preventing excessive electronic conductivity and maintaining stability with lithium metal. This parameter optimization resolves the contradiction by finding the optimal point in the temperature range that balances crystallinity formation with stability preservation.

Inventive Principle:
Principle #35Parameter changes

2Stability of the object's composition

If heat treatment temperature is increased to achieve high crystallinity, then crystallinity is improved, but electronic conductivity increases causing side reactions

Engineering Contradiction:
ImprovecrystallinityVSAvoidelectronic conductivity
Core Design Contradiction:
Stability of the object's compositionVSObject-generated harmful factors

Solution Approach 1:

The patent controls the heat treatment temperature within a specific range (400-500°C) to achieve sufficient crystallinity while limiting electronic conductivity to acceptable levels. This parameter control prevents the harmful effect of excessive electronic conductivity that would cause side reactions, while still obtaining the desired crystalline structure.

Inventive Principle:
Principle #35Parameter changes

3Ease of manufacture

If amorphous sulfide-based solid electrolyte is used to reduce manufacturing temperature, then manufacturing cost is reduced, but reactivity with lithium metal increases

Engineering Contradiction:
Improvemanufacturing temperatureVSAvoidreactivity with lithium metal
Core Design Contradiction:
Ease of manufactureVSReliability

Solution Approach 1:

The patent applies heat treatment at optimized temperatures (400-500°C) to transform the amorphous structure into a crystalline structure. This parameter change reduces the reactivity with lithium metal while maintaining manufacturing feasibility, as the heat treatment can be performed in standard equipment without requiring excessively high temperatures.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent utilizes the phase transition from amorphous to crystalline state through controlled heat treatment. This phase transition fundamentally changes the material properties, reducing reactivity with lithium metal while maintaining the benefits of lower manufacturing temperatures compared to traditional high-temperature crystallization methods.

Inventive Principle:
Principle #36Phase transitions

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 provides a stable, high-crystallinity sulfide-based solid electrolyte with excellent lithium ion conductivity and low electronic conductivity, reducing the risk of short circuits and enabling efficient operation of all-solid-state batteries without the need for H2S gas.

Implementation Method 1

ions other than Li ions in such a solid electrolyte do not move, side reactions due to the movement of anions do not occur

Methodology Applied
Scientific EffectIonic conduction: Conduction (electrical)

Implementation Method 2

having low electronic conductivity while having excellent ionic conductivity

Methodology Applied
Scientific EffectElectronic conductivity: Conduction (electrical)

Implementation Method 3

heat treatment at a temperature of 500° C. or higher to achieve high crystallinity

Methodology Applied
Scientific EffectHeat treatment: Heat Treatment

Implementation Method 4

a crystalline sulfide-based solid electrolyte that has excellent ion conductivity, low electronic conductivity and excellent stability with respect to a lithium metal while having high crystallinity

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Data Source

PatentUS20230378524A1Sulfide-based solid electrolyte for all-solid lithium secondary battery and method for preparing sulfide-based solid electrolyte
Publication Date: 2023.11.23 POSCO JK SOLID SOLUTION CO LTD

AI summary

The present invention relates to a sulfide-based solid electrolyte for an all-solid lithium secondary battery, and to a method for preparing the sulfide-based solid electrolyte. The present invention has an effect of providing a sulfide-based solid electrolyte that has excellent stability with respect to lithium metal and has excellent ion conductivity, while having high crystallinity. The present invention has an effect of providing a method for preparing a sulfide-based solid electrolyte that has excellent stability with respect to lithium metal and has excellent ion conductivity, while having high crystallinity even when heat-treated at a low temperature.