Nanofiber Polymer Composite Electrolytes for Low-Resistance Solid-State Cells

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Solution Overview

Problem

Current solid-state lithium lanthanum zirconium oxide (LLZO) electrolytes in batteries face issues with high interfacial resistance, mechanical failures, and poor workability due to high temperature sintering, leading to suboptimal electrode electrolyte contact and limited scalability in manufacturing.

Innovation Solution

The development of ceramic lithium-conducting nanofibers integrated with polymer electrolytes, specifically using LLZO-PEO composite thin films, to enhance ionic conductivity and electrochemical stability, with nanofibers forming a three-dimensional network for improved ion transport and mechanical robustness.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Stability of the object's composition

If high temperature sintering (>1100°C) is used to process LLZO powders, then the ceramic particles achieve sufficient density and stability, but the interfacial resistance increases, grain size becomes large, and mechanical failures occur

Engineering Contradiction:
Improveceramic particle density and stabilityVSAvoidinterfacial resistance and mechanical strength
Core Design Contradiction:
Stability of the object's compositionVSReliability

Solution Approach 1:

The patent changes the processing temperature parameter from conventional high temperature (>1100°C) to low temperature (900-1100°C) sintering, which fundamentally alters the microstructure development. This temperature reduction prevents excessive grain growth and facet formation while still achieving sufficient ceramic density, thereby resolving the contradiction between stability and reliability

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent creates a composite material system combining LLZO ceramic particles with polymer matrix (forming CPEs). This composite structure allows the ceramic to provide stability and ionic conductivity while the polymer provides flexibility and good interfacial contact, thus resolving the mechanical fragility and high interfacial resistance issues associated with pure ceramic electrolytes

Inventive Principle:
Principle #40Composite materials

2Ease of manufacture

If conventional sintering methods are used, then ceramic particles are formed, but the grain morphology becomes facet-shaped with poor electrode electrolyte contact

Engineering Contradiction:
Improveceramic particle formationVSAvoidgrain morphology and interfacial contact quality
Core Design Contradiction:
Ease of manufactureVSManufacturing precision

Solution Approach 1:

The patent modifies the sintering temperature parameter to a lower range (900-1100°C) which changes the grain growth kinetics. This prevents the formation of large facet-shaped grains and instead produces finer, more equiaxed grains with better surface area contact to electrodes, improving interfacial contact quality while maintaining manufacturability

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent optimizes the local microstructure by controlling grain size and morphology through temperature adjustment. The resulting fine-grained structure provides numerous grain boundaries and surfaces for electrode contact, creating locally optimized interfaces throughout the electrolyte that enhance overall electrochemical performance

Inventive Principle:
Principle #3Local quality

3Stability of the object's composition

If high temperature sintering is applied, then ceramic electrolytes achieve structural stability, but workability and scalability for real-world manufacturing deteriorate

Engineering Contradiction:
Improveelectrolyte structural stabilityVSAvoidworkability and manufacturing scalability
Core Design Contradiction:
Stability of the object's compositionVSEase of manufacture

Solution Approach 1:

The patent reduces the sintering temperature from >1100°C to 900-1100°C, which significantly lowers the energy input and processing complexity required. This temperature reduction makes the manufacturing process more scalable and easier to implement in real-world production while still achieving sufficient structural stability of the ceramic electrolyte

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

By forming composite polymer electrolytes that combine ceramic particles with polymer matrix, the patent creates a material that is easier to process and manufacture. The polymer component provides processability and flexibility during manufacturing, while the ceramic phase maintains structural stability, thus resolving the contradiction between stability and ease of manufacture

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

This approach results in high-energy-density, fast-charging solid-state lithium batteries with reduced mechanical fractures and improved scalability, enabling advanced performance for increased market adoption.

Implementation Method 1

The nanofibers provide Li-ion transport channels to enable fast-charging capabilities

Methodology Applied
Scientific EffectIon conduction: Conduction (electrical)

Implementation Method 2

An electrospinning process is used to form nanofibers

Methodology Applied
Scientific EffectElectrospinning: Electrohydrodynamics

Implementation Method 3

The precursor nanofibers are then annealed or sintered at a relatively low temperature (e.g., 600 to 800° C.) to form c-LLZO nanofibers

Methodology Applied
Scientific EffectAnnealing: Annealing

Data Source

PatentUS11923501B2Solid-state nanofiber polymer multilayer composite electrolytes and cells
Publication Date: 2024.03.05 UCHICAGO ARGONNE LLC
  • US11923501B2 patent drawing
  • US11923501B2 patent drawing
  • US11923501B2 patent drawing

AI summary

A solid-state electrolyte for a multilayer solid-state electrochemical cell is described herein. The electrolyte comprises a lithium electrolyte salt and nanofibers of a cubic phase lithium lanthanum zirconium oxide (c-LLZO), and a polymer interspersed with the nanofibers and electrolyte salt. Electrochemical cells comprising the solid-state electrolyte, and solid-state cathodes comprising the nanofibers of c-LLZO are also described herein.