Crystallized glass and method for manufacturing crystallized glass

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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, an element M (such as zirconium, hafnium, tin, samarium, niobium, tantalum, tungsten, or molybdenum), phosphorus, oxygen, and optionally boron or silicon, with a monoclinic crystal structure peak at 2θ=20° to 30° and a half width of 0.10° or more, produced through a method involving mixing, heating, cooling, and crystallization.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If oxide-based solid electrolyte is used, 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 material system consisting of Li-M-P-O glass ceramic with specific monoclinic crystal structure. The composite nature of the material (combining glass matrix with crystalline phases containing Li, M, P, O) enables simultaneous achievement of high environmental stability inherent to oxides and enhanced lithium ion conductivity through the specific crystal structure, resolving the contradiction between stability and conductivity.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The invention changes the structural parameters of the oxide-based electrolyte by controlling the formation of monoclinic crystal structure with specific XRD peak characteristics (2θ=20°-30°, half-width ≥0.10°). By adjusting compositional parameters (Li, M, P, O ratios) and thermal processing parameters (heating to 1200°C-1650°C), the material achieves optimal lithium ion conductivity while maintaining oxide environmental stability.

Inventive Principle:
Principle #35Parameter changes

2Object-generated harmful factors

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

Engineering Contradiction:
Improvelithium ion conductivityVSAvoidenvironmental stability
Core Design Contradiction:
Object-generated harmful factorsVSReliability

Solution Approach 1:

The Li-M-P-O glass ceramic with monoclinic crystal structure serves as an oxide-based composite material that achieves sulfide-level conductivity (0.40 mS/cm or more) while maintaining oxide environmental stability. The specific crystal structure and compositional design enable this material to bridge the performance gap between sulfide and oxide electrolytes.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

By changing the chemical composition parameters (incorporating specific elements M such as Ta, Nb, W, Mo) and thermal processing parameters (heating temperature 1200°C-1650°C), the invention transforms the oxide-based material properties to achieve high lithium ion conductivity comparable to sulfides, while retaining the environmental stability advantage of oxides.

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 lithium ion conductivity of 0.40 mS/cm or more, suitable for use as a solid electrolyte in lithium ion batteries, addressing the conductivity gap in existing oxide-based electrolytes.

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 EffectFreezing: Freezing

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

PatentUS20250243107A1Crystallized glass and method for manufacturing crystallized glass
Publication Date: 2025.07.31 AGC INC
  • US20250243107A1 patent drawing
  • US20250243107A1 patent drawing
  • US20250243107A1 patent drawing

AI summary

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