Garnet Oxide Electrolyte Composition With High Li-Ion Conductivity

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Solution Overview

Problem

The preparation of raw materials and firing methods for producing garnet-type oxide with Li, Zr, and La must be rigorously controlled to stabilize the cubic system, making the process complex and difficult to manage.

Innovation Solution

An oxide with a garnet-type crystal structure including Li, La, and Zr, where the crystal structure belongs to the space group I4 1 /acd, with a Li occupancy of 8a sites ranging from 30% to 95% and 16e sites occupancy of 60% or less, is developed. This oxide can be produced through a simpler method, and optional Sr can be included to enhance stability and ion conductivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Stability of the object's composition

If rigorous control of raw material preparation and firing method is applied to stabilize the cubic system, then the stability of the oxide is improved, but the manufacturing complexity increases

Engineering Contradiction:
Improvestability of cubic systemVSAvoidmanufacturing process complexity
Core Design Contradiction:
Stability of the object's compositionVSDevice complexity

Solution Approach 1:

The invention changes the crystal system parameter from cubic to tetragonal (space group I41/acd), which fundamentally alters the stability mechanism. This parameter change allows the oxide to achieve stability without requiring rigorous control of raw material preparation and firing methods, thus resolving the contradiction between stability and manufacturing complexity

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

Instead of attempting to stabilize the conventional cubic system through rigorous process control, the invention inverts the approach by deliberately adopting a tetragonal crystal system that inherently provides stability through its unique Li occupancy configuration (8a sites: 30-95%, 16e sites: 60% or less), thereby simplifying the manufacturing process while maintaining stability

Inventive Principle:
Principle #13The other way round (Inversion)

2Ease of manufacture

If conventional tetragonal LLZ is used, then the manufacturing process is simpler, but the ion conductivity is lower

Engineering Contradiction:
Improveease of productionVSAvoidion conductivity
Core Design Contradiction:
Ease of manufactureVSReliability

Solution Approach 1:

The invention applies local quality by specifically controlling the Li occupancy at different crystallographic sites (8a sites: 30-95%, 16e sites: 60% or less) within the tetragonal structure. This localized control of Li distribution at specific sites enhances ion conductivity while maintaining the simplicity of the tetragonal manufacturing process, resolving the contradiction between ease of manufacture and ion conductivity

Inventive Principle:
Principle #3Local quality

Solution Approach 2:

The invention creates a composite-like structure within the tetragonal LLZ by optimizing the combination of Li occupancies at 8a and 16e sites, effectively combining the manufacturing simplicity of tetragonal systems with the high ion conductivity characteristics typically associated with cubic systems

Inventive Principle:
Principle #40Composite materials

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 simplified production method allows for the easy fabrication of an oxide with high ion conductivity, achieving ion conductivity of 10 -4 S/cm or higher at room temperature, which is 100 times greater than that of conventional tetragonal LLZ, while maintaining stability and ease of production.

Implementation Method 1

an oxide which has a garnet-type crystal structure including Li, Zr, and La exhibits high chemical stability and a lithium ion-conductive property

Methodology Applied
Scientific EffectIon conduction: Conduction (electrical)

Data Source

PatentEP4566997A1Oxide, electrolyte composition, and electricity storage device
Publication Date: 2025.06.11 NITERRA CO LTD
  • EP4566997A1 patent drawingFigure 1
  • EP4566997A1 patent drawingFigure 2
  • EP4566997A1 patent drawingFigure 3

AI summary

Provided are an oxide which can be produced by a simple method, an electrolyte composition, and an electricity storage device. The oxide has a garnet-type crystal structure including Li, La, and Zr. The crystal structure belongs to the space group I41/acd and has an Li occupancy rate at the 8a site of 30-95% and an Li occupancy rate at the 16e site of 60% or less (excluding 0%). The oxide can contain Sr. The electrolyte composition and the electricity storage device include the oxide.