Free-Standing Sulfide Electrolyte Sheets With Slurry-Calendered Densification

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Solution Overview

Problem

Existing methods for manufacturing sulfide-based, free-standing sheet-type solid-state electrolytes face challenges such as high pressure requirements, poor mechanical properties, and difficulty in controlling microstructure, leading to limited scalability and inhomogeneous distribution of binder and sulfide particles, which hinder their integration into industrial battery manufacturing processes.

Innovation Solution

A method involving mixing a sulfide ion conductor material with a non-polar or low-polar binder in a solvent, spreading the mixture onto a substrate, calendering to densify, and drying under vacuum to form a flexible, free-standing sheet-type electrolyte with excellent mechanical strength and ionic conductivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If sulfide SE membranes are formed by grinding sulfide material into fine powder, mixing with thermoplastic polymer binder, and pressing into sheet, then sheet-type electrolyte can be obtained, but the microstructure control is difficult and binder and sulfide particles are inhomogeneously distributed

Engineering Contradiction:
Improvesheet-type electrolyte formationVSAvoidmicrostructure control and particle distribution
Core Design Contradiction:
Ease of manufactureVSManufacturing precision

Solution Approach 1:

The patent changes the processing parameters by using a slurry-based approach with specific solvent systems and controlled drying conditions instead of direct pressing of dry powders. This allows for better control of microstructure and homogeneous particle distribution while maintaining ease of manufacture

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent introduces a slurry medium as an intermediary between the sulfide powder and binder, allowing for better dispersion and distribution of particles before final formation. The slurry acts as a carrier that enables homogeneous mixing and controlled deposition

Inventive Principle:
Principle #24Intermediary (Mediator)

2Reliability

If pelletizing sulfide SEs is used in laboratory research, then electrolyte samples can be obtained, but the pressures required approach prohibitive levels when scaled up

Engineering Contradiction:
Improveelectrolyte sample qualityVSAvoidpressing pressure
Core Design Contradiction:
ReliabilityVSStress or pressure

Solution Approach 1:

The patent replaces the high-pressure mechanical pelletizing system with a low-pressure slurry casting system. Instead of using extreme pressures to form dense pellets, the method uses a liquid slurry that can be deposited and dried at much lower pressures, maintaining electrolyte quality while enabling scale-up

Inventive Principle:
Principle #28Mechanics substitution (Replace mechanical system)

Solution Approach 2:

The patent utilizes phase transitions by working with the binder in a softened or molten state during slurry preparation, then allowing it to solidify during drying. This phase change enables formation at low pressure that would be impossible with cold-pressing alone

Inventive Principle:
Principle #36Phase transitions

3Ease of manufacture

If sulfide SE pellets are used, then electrolyte can be formed, but their poor mechanical properties result in finite lower bound on thickness which limits cell-based energy densities

Engineering Contradiction:
Improveelectrolyte formationVSAvoidmechanical properties
Core Design Contradiction:
Ease of manufactureVSStrength

Solution Approach 1:

The patent creates a composite material system where sulfide particles are embedded in a polymer binder matrix. This composite structure combines the high ionic conductivity of sulfides with the mechanical flexibility of polymers, enabling thin-film formation with adequate mechanical strength

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent produces flexible thin-film electrolytes by using the slurry casting method followed by controlled drying. The resulting free-standing films can be made much thinner than pressed pellets while maintaining mechanical integrity, enabling higher energy densities

Inventive Principle:
Principle #30Flexible shells and thin films

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 enables the production of thin, flexible, and mechanically robust sulfide-based solid-state electrolytes suitable for battery cells, with improved ionic conductivity and compatibility with industrial roll-to-roll processes.

Implementation Method 1

mixing a sulfide ion conductor-containing material and a binder in a solvent to obtain a slurry composition

Methodology Applied
Scientific EffectSolvation: Solvation

Implementation Method 2

disposing the slurry composition onto a planar substrate. The method further includes spreading the slurry composition on the substrate

Methodology Applied
Scientific EffectDeposition: Deposition (physical)

Implementation Method 3

calendering the film to densify the film

Methodology Applied
Scientific EffectCompression: Compression

Implementation Method 4

drying the film under vacuum

Methodology Applied
Scientific EffectEvaporation: Evaporation

Data Source

PatentUS20250239649A1Free-standing sulfide solid electrolyte separators
Publication Date: 2025.07.24 UT BATTELLE LLC
  • US20250239649A1 patent drawing
  • US20250239649A1 patent drawing
  • US20250239649A1 patent drawing

AI summary

A method of manufacturing a free-standing, sheet-type solid-state electrolyte is provided. The method includes: mixing a sulfide ion conductor-containing material and a non-polar or low-polar binder in a solvent to obtain a slurry composition; disposing the slurry composition onto a planar substrate; spreading the slurry composition on the substrate to obtain a film; calendering the film to densify the film; and subsequently drying the film under vacuum. The binder may be polyisobutylene and may be present in the slurry composition in an amount of up to 10 wt. %, optionally between 1 and 5 wt. %. The sulfide ion conductor-containing material may be a lithium argyrodite having the chemical formula Li6PS5X in which X is Cl, Br, or I. The solvent may be toluene or xylene. The film may have a thickness of between 10 and 200 μm.