Crystallized Glass Electrolyte Composition for Higher Li-Ion Conductivity

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Solution Overview

Problem

Current oxide-based solid electrolytes for lithium ion batteries have low lithium ion conductivity, which is not comparable to sulfide-based solid electrolytes, and there is a need for an oxide-based solid electrolyte with higher lithium ion conductivity.

Innovation Solution

A glass ceramic composed of lithium (Li), an element M (zirconium (Zr), hafnium (Hf), tin (Sn), samarium (Sm), niobium (Nb), tantalum (Ta), tungsten (W), or molybdenum (Mo), phosphorus (P), oxygen (O), and optionally boron (B) or silicon (Si), with a monoclinic crystal structure peak at 2θ = 20° to 30° and a half width of 0.10° or more, produced through mixing, melting, cooling, pulverizing, and heat treatment to form a glass ceramic.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If oxide-based solid electrolyte is used instead of sulfide-based solid electrolyte, then environmental stability and ease of handling are improved, but lithium ion conductivity deteriorates

Engineering Contradiction:
Improveenvironmental stabilityVSAvoidlithium ion conductivity
Core Design Contradiction:
ReliabilityVSObject-generated harmful factors

Solution Approach 1:

The invention uses a composite glass ceramic material containing Li-M-P-O crystalline phase embedded in a glass matrix. This composite structure combines the high environmental stability of oxide-based materials with enhanced lithium ion conductivity through the crystalline phase, achieving both improved reliability and reduced harmful effects.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The invention changes the chemical composition parameters by incorporating specific elements (M = Zr, Hf, Sn, Sm, Nb, Ta, W, or Mo) and controlling the ratios of Li, P, and O. It also changes the physical state from amorphous to crystalline glass ceramic, and optimizes the half width of the maximum peak (0.10° or more) to achieve high lithium ion conductivity while maintaining environmental stability.

Inventive Principle:
Principle #35Parameter changes

2Ease of manufacture

If conventional oxide-based solid electrolyte composition is used, then ease of manufacture is improved, but lithium ion conductivity deteriorates

Engineering Contradiction:
ImprovemanufacturabilityVSAvoidlithium ion conductivity
Core Design Contradiction:
Ease of manufactureVSObject-generated harmful factors

Solution Approach 1:

The invention optimizes composition parameters (Li, M, P, O ratios) and processing parameters (heating temperature 1200-1650°C, cooling rate, crystallization temperature) to achieve high lithium ion conductivity. The specific requirement of half width ≥0.10° provides a clear manufacturing target that balances performance with manufacturability.

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 glass ceramic achieves a high lithium ion conductivity of 0.40 mS/cm, suitable for use as a solid electrolyte in lithium ion batteries, enhancing battery performance.

Implementation Method 1

heating the mixed powder to a temperature of 1200°C to 1650°C to obtain a melt

Methodology Applied
Scientific EffectMelting: Melting

Implementation Method 2

cooling the melt to form a glass cullet containing a seed crystal

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Implementation Method 3

heating the glass frit to a temperature equal to or higher than a crystallization temperature to form a glass ceramic

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Data Source

PatentEP4592259A1Crystallized glass and method for manufacturing crystallized glass
Publication Date: 2025.07.30 AGC INC
  • EP4592259A1 patent drawingFigure 1
  • EP4592259A1 patent drawingFigure 2
  • EP4592259A1 patent drawingFigure 3

AI summary

A crystallized glass comprising: lithium (Li), element M, phosphorus (P), and oxygen (O); and at least one selected from boron (B) and silicon (Si), wherein the element M includes at least one selected from the group consisting of zirconium (Zr), hafnium (Hf), tin (Sn), samarium (Sm), niobium (Nb), tantalum (Ta), tungsten (W), and molybdenum (Mo), the maximum peak, in an X-ray diffraction pattern of the crystallized glass, appearing in a range of 2θ=20° to 30° is derived from a monoclinic crystal structure, and the half width of the maximum peak is 0.10° or more.