Lithium Solid Electrolyte Film Processing for Cubic Phase Control

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Solution Overview

Problem

Current methods for manufacturing garnet-type lithium solid electrolytes are not scalable and economically viable, and they struggle to stabilize the cubic phase with desirable lithium ion conductivity, which is essential for solid-state lithium-ion batteries.

Innovation Solution

A method involving a composition of lithium, lanthanum, and zirconium precursors is used to form a film on a substrate at 270° C. to 500° C., followed by heat-treating at 300° C. to 750° C. for 1 to 100 hours to produce a lithium solid electrolyte with reduced local stress, stabilizing the cubic phase and enhancing conductivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If conventional bulk-type sintering methods are used to manufacture garnet-type lithium solid electrolytes, then the material can achieve desired lithium ion conductivity, but the manufacturing process is not scalable and economically viable

Engineering Contradiction:
Improvelithium ion conductivityVSAvoidscalability and economic viability
Core Design Contradiction:
ReliabilityVSEase of manufacture

Solution Approach 1:

The bulk sintering process is segmented into thin-film deposition followed by low-temperature heat treatment. The electrolyte is manufactured as a thin film on a substrate rather than as a bulk material, enabling scalable production while maintaining desired conductivity properties through controlled film formation and phase stabilization.

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The manufacturing parameters are fundamentally changed from high-temperature bulk sintering to low-temperature thin-film heat treatment (300-750°C). This parameter change enables scalable production by reducing energy consumption and allowing integration with substrate-based manufacturing processes, while still achieving the desired cubic phase and conductivity.

Inventive Principle:
Principle #35Parameter changes

2Reliability

If high heat treatment temperatures (above 750°C) are used to stabilize the cubic phase, then lithium ion conductivity improves, but manufacturing complexity and energy consumption increase

Engineering Contradiction:
Improvecubic phase stability and conductivityVSAvoidmanufacturing process complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The cubic phase is stabilized through preliminary compositional design (doping with Al, Ga, Ca, or Mg) before heat treatment. This preliminary action allows the material to achieve cubic phase stability at lower temperatures (300-750°C) rather than requiring high-temperature processing, thereby reducing manufacturing complexity while maintaining desired properties.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The heat treatment temperature parameter is reduced from conventional high temperatures (>750°C) to a lower range (300-750°C). This parameter change is enabled by compositional modifications that stabilize the cubic phase, simplifying the manufacturing process while achieving the desired phase stability and conductivity.

Inventive Principle:
Principle #35Parameter changes

3Reliability

If long heat treatment times (100 hours) are used to achieve high crystallinity, then lithium ion conductivity improves, but production efficiency decreases

Engineering Contradiction:
Improvecrystallinity and conductivityVSAvoidproduction efficiency
Core Design Contradiction:
ReliabilityVSProductivity

Solution Approach 1:

The heat treatment is applied periodically in controlled cycles rather than as a continuous long-duration process. The periodic heat treatment at optimized temperatures (300-750°C) achieves high crystallinity and conductivity in 1-100 hours by maintaining optimal conditions throughout the process, improving production efficiency compared to conventional extended heat treatments.

Inventive Principle:
Principle #19Periodic action

Solution Approach 2:

The heat treatment temperature parameter is optimized to a specific range (300-750°C) that accelerates crystallization kinetics. This parameter change allows high crystallinity to be achieved in shorter times (1-100 hours) rather than requiring extremely long treatment durations, thereby improving production efficiency while maintaining desired conductivity.

Inventive Principle:
Principle #35Parameter changes

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 method achieves high crystallinity and improved lithium-ion conductivity, reducing local stress and lattice strain, thereby stabilizing the cubic phase and enhancing ion transport, making it suitable for scalable production.

Implementation Method 1

heat-treating the film at 300° C. to less than 750° C. for 1 hour to 100 hours to manufacture the lithium solid electrolyte

Methodology Applied
Scientific EffectHeat treatment: Heat Treatment

Implementation Method 2

Garnet-type oxides can provide promising lithium-ion conductivity

Methodology Applied
Scientific EffectLithium-ion conductivity: Conduction (electrical)

Data Source

PatentUS11757127B2Lithium solid electrolyte and method of manufacture thereof
Publication Date: 2023.09.12 SAMSUNG ELECTRONICS CO LTD
  • US11757127B2 patent drawing
  • US11757127B2 patent drawing
  • US11757127B2 patent drawing

AI summary

A method of manufacturing a lithium solid electrolyte, the method including: providing a composition including a lithium precursor, a lanthanum precursor, and a zirconium precursor; disposing the composition on a substrate having a temperature of 270° C. to 500° C. to form a film; and heat-treating the film at 300° C. to less than 750° C. for 1 hour to 100 hours to manufacture the lithium solid electrolyte.