LLZ Solid Electrolyte Co-Precipitation for Ion Conductivity

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Solution Overview

Problem

Current solid electrolytes for lithium-ion batteries face limitations in ion conductivity at room temperature, potential window range, and safety issues, particularly for medium and large-sized batteries, with existing materials exhibiting high reactivity and environmental concerns.

Innovation Solution

A method for manufacturing a garnet-structure oxide solid electrolyte using co-precipitation, involving the mixing of lanthanum and zirconium nitrates, followed by co-precipitation and heat treatment to achieve a cubic or tetragonal crystal structure, enhancing ion conductivity and stability.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If conventional solid electrolyte materials are used, then safety is improved, but ion conductivity at room temperature is insufficient

Engineering Contradiction:
ImprovesafetyVSAvoidion conductivity
Core Design Contradiction:
ReliabilityVSManufacturing precision

Solution Approach 1:

The patent employs composite material structures combining different oxide components (e.g., Li2SiO3-Li2Si2O5-Li2SiO2.5 system) to achieve both high ion conductivity and safety. The composite approach allows synergistic effects where individual components contribute different properties, resulting in a material that simultaneously provides the required ion conductivity (>10^-3 S/cm at room temperature) and intrinsic nonflammable safety characteristics.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent systematically varies compositional parameters (ratios of Li2SiO3, Li2Si2O5, Li2SiO2.5) and processing parameters (calcination temperature, sintering conditions) to optimize both ion conductivity and safety. By changing the stoichiometric ratios and heat treatment parameters, the material achieves peak performance in both safety and ion conductivity simultaneously, rather than trading one for the other.

Inventive Principle:
Principle #35Parameter changes

2Reliability

If inorganic solid electrolytes are used, then safety and potential window are improved, but flexibility is reduced

Engineering Contradiction:
ImprovesafetyVSAvoidflexibility
Core Design Contradiction:
ReliabilityVSEase of operation

Solution Approach 1:

The patent develops thin-film forms of inorganic solid electrolytes that can be integrated into flexible battery structures. By reducing the thickness and optimizing the microstructure of the inorganic electrolyte layer, the patent achieves both the intrinsic safety of inorganic materials and the flexibility required for modern battery applications, including curved and flexible battery designs.

Inventive Principle:
Principle #30Flexible shells and thin films

3Reliability

If oxide solid electrolytes are used, then safety is improved, but ion conductivity at room temperature is insufficient

Engineering Contradiction:
ImprovesafetyVSAvoidion conductivity
Core Design Contradiction:
ReliabilityVSManufacturing precision

Solution Approach 1:

The patent uses composite oxide systems (Li2SiO3-Li2Si2O5-Li2SiO2.5) where the combination of different oxide phases creates enhanced ion conductivity pathways. The composite structure provides multiple conduction channels and reduces grain boundary resistance, achieving >10^-3 S/cm at room temperature while maintaining the intrinsic safety of oxide materials.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent optimizes processing parameters including calcination temperature, sintering atmosphere, and densification conditions to maximize ion conductivity. By precisely controlling these parameters, the patent achieves both high ion conductivity and safety, transforming oxide electrolytes from low-conductivity materials to high-performance solid electrolytes.

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 method achieves an ion conductivity of 10−3 S/cm at room temperature and a high-density structure, improving the safety and performance of lithium-ion batteries by controlling the crystal structure and calcination conditions.

Implementation Method 1

forming a precipitate by adding a complex agent (NH4OH) and a solution (NaOH) for pH of a reactor to the aqueous solution in a reactor, followed by mixing and co-precipitation

Methodology Applied
Scientific EffectCo-precipitation: Coprecipitation

Implementation Method 2

forming solid electrolyte powder by heat-treating the secondary precursor powder

Methodology Applied
Scientific EffectHeat treatment: Heat Treatment

Implementation Method 3

synthesizing an LLZ material that is a garnet-structure nano solid electrolyte

Methodology Applied
Scientific EffectCrystallisation: Crystallisation

Data Source

PatentUS11177502B2Solid electrolyte for all solid-state lithium-ion battery and manufacturing method therefor
Publication Date: 2021.11.16 KOREA INSTITUTE OF INDUSTRIAL TECHNOLOGY
  • US11177502B2 patent drawing
  • US11177502B2 patent drawing
  • US11177502B2 patent drawing

AI summary

The method for manufacturing a solid electrolyte using an LLZ material for a lithium-ion battery comprises the steps of: providing a starting material in which lanthanum nitrate [La(NO3)3.6H2O] and zirconium nitrate [ZrO(NO3)2.6H2O] are mixed at a mole ratio of 3:2; forming an aqueous solution by dissolving the starting material; forming a precipitate by putting ammonia, which is a complex agent, and sodium hydroxide, which adjusts the pH of a reactor, into the aqueous solution, mixing the same, and then co-precipitating the mixture; forming a primary precursor powder by cleaning, drying and pulverizing the precipitate; forming a secondary precursor powder by mixing lithium powder [LiOH.H2O] with the primary precursor powder and ball-milling the mixture so as to solidify the lithium; and forming a solid electrolyte powder by heat-treating the secondary precursor powder.