Three-Layer Composite Electrolyte for Flexible Solid-State Battery Films

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Solution Overview

Problem

Conventional oxide-based solid electrolytes lack flexibility and require high processing costs for large-area production, and garnet-based electrolytes face issues with poor interfacial contact and brittleness, making them difficult to use in thin and flexible film applications.

Innovation Solution

A three-layer structure composite electrolyte is developed, comprising a garnet dominant-composite solid electrolyte (GD-CSE) as the center layer and ionic polymer interlayers (IPI) on both sides, with specific compositions and additives to enhance mechanical strength and ionic conductivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If garnet-based oxide solid electrolyte is used, then high ionic conductivity and electrochemical stability are achieved, but poor interfacial contact and brittleness occur

Engineering Contradiction:
Improveionic conductivityVSAvoidmechanical flexibility
Core Design Contradiction:
ReliabilityVSStrength

Solution Approach 1:

The invention creates a composite solid electrolyte by combining garnet-based oxide particles (70-90 wt%) with polymer matrix (10-30 wt%). This composite structure integrates the high ionic conductivity of ceramic garnet with the mechanical flexibility and adhesive properties of polymer, resolving the contradiction between reliability and strength.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The invention optimizes the weight ratio of ceramic to polymer within specific ranges (70-90 wt% ceramic, 10-30 wt% polymer) to balance ionic conductivity and mechanical properties. Additionally, controlling particle size (0.5-20 μm) and adding plasticizers modify the physical parameters to achieve both high conductivity and flexibility.

Inventive Principle:
Principle #35Parameter changes

2Reliability

If high content ceramic filler is added to polymer matrix, then ionic conductivity is improved, but filler aggregation occurs which lowers ionic conductivity

Engineering Contradiction:
Improveionic conductivityVSAvoidhomogeneity
Core Design Contradiction:
ReliabilityVSStability of the object's composition

Solution Approach 1:

The invention utilizes porous polymer matrices with controlled pore sizes that can accommodate ceramic particles. The porous structure prevents filler aggregation by providing adequate spacing and distribution channels, maintaining homogeneity while allowing high ceramic content (70-90 wt%) for high ionic conductivity.

Inventive Principle:
Principle #31Porous materials

Solution Approach 2:

The invention controls particle size parameters (0.5-20 μm) and uses specific surface area characteristics to prevent aggregation. By optimizing these physical parameters, the ceramic filler distributes uniformly in the polymer matrix, achieving both high ionic conductivity and compositional stability.

Inventive Principle:
Principle #35Parameter changes

3Reliability

If ceramic solid electrolyte is used for thin film formation, then high safety is achieved, but poor interfacial contact and thickness control make practical use difficult

Engineering Contradiction:
ImprovesafetyVSAvoidthin film formation
Core Design Contradiction:
ReliabilityVSEase of manufacture

Solution Approach 1:

The polymer matrix component enables the formation of flexible thin films containing ceramic particles. The polymer's processability allows for creating thin, uniform films (controlling thickness) while maintaining the high safety characteristics of ceramic electrolytes, resolving the manufacturing difficulty.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The composite structure combines ceramic safety with polymer processability. The polymer matrix provides ease of manufacturing into thin films with good interfacial contact, while the ceramic filler maintains high safety, achieving both reliability and ease of manufacture.

Inventive Principle:
Principle #40Composite materials

4Strength

If polymer electrolyte is used, then mechanical flexibility and adhesive properties are achieved, but low ionic conductivity at room temperature occurs

Engineering Contradiction:
Improvemechanical flexibilityVSAvoidionic conductivity
Core Design Contradiction:
StrengthVSReliability

Solution Approach 1:

The invention creates a composite where polymer provides mechanical flexibility and adhesion, while embedded ceramic garnet particles provide high ionic conductivity. This composite structure resolves the contradiction by combining the complementary strengths of both materials.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The invention optimizes the polymer-to-ceramic ratio (10-30 wt% polymer, 70-90 wt% ceramic) to ensure sufficient ceramic content for high ionic conductivity while maintaining enough polymer for mechanical flexibility. Additional parameter optimization including particle size and plasticizer content further enhances ionic 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 composite electrolyte achieves high ionic conductivity (0.5 to 1.2 mS/cm), excellent electrochemical stability (up to 5.0 V versus Li/Li+), and flexibility, suitable for large-area production and practical use in all-solid-state batteries.

Implementation Method 1

an ionic polymer interlayer (IPI) disposed on both sides of the solid electrolyte center layer... lithium ion conductivity of the three-layer structure-CSE can be improved by introducing an IPI layer

Methodology Applied
Scientific EffectIon conduction: Conduction (electrical)

Implementation Method 2

a plastic crystal electrolyte (PCE, LiTFSI dolven succinonitrile, 15 wt. %) as an ionic-conductive additive... can be improved by introducing an IPI layer

Methodology Applied
Scientific EffectIon conduction: Conduction (electrical)

Data Source

PatentUS20250239645A1Oxide-based three-layer structure composite electrolyte and all-solid-state battery using the same
Publication Date: 2025.07.24 KOREA INST OF ENERGY RES
  • US20250239645A1 patent drawing
  • US20250239645A1 patent drawing
  • US20250239645A1 patent drawing

AI summary

An embodiment of the present invention provides a three-layer structure composite electrolyte including an oxide-based solid electrolyte center layer (CSE, composite solid electrolyte); and an ionic polymer interlayer (IPI) disposed on both sides of the solid electrolyte center layer.