c-LLZO Solid Electrolyte Films With Metal Oxide Lithium Interface

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Solution Overview

Problem

Conventional methods for producing thin films of cubic Li7La3Zr2O12 (c-LLZO) for solid-state lithium batteries are energy-intensive, environmentally unfriendly, and result in non-uniform particle sizes, limiting their effectiveness in achieving high ionic conductivity and safety in lithium batteries.

Innovation Solution

A method involving flame-assisted spray pyrolysis of inorganic precursors dissolved in organic solvents to generate aerosols, which are converted to solid powders at elevated temperatures and annealed to produce c-LLZO particles with a narrow size range (20 nm to 10 μm) suitable for thin films (5-50 μm) using a more economical and environmentally friendly process.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Use of energy by stationary object

If conventional methods are used to produce thin films of cubic Li7La3Zr2O12, then the production process is energy-intensive and environmentally unfriendly, but the method can still produce solid electrolyte particles

Engineering Contradiction:
Improveenergy consumptionVSAvoidenvironmental harm
Core Design Contradiction:
Use of energy by stationary objectVSObject-generated harmful factors

Solution Approach 1:

The patent changes the production parameters by using flame-assisted spray pyrolysis instead of conventional solid-state reaction methods. This involves dissolving inorganic precursors (lithium nitrate, lanthanum nitrate, zirconium nitrate) in organic solvents to create a precursor solution, which is then sprayed and pyrolyzed in a flame to form uniform c-LLZO particles with narrow size distribution (20 nm to 10 μm), eliminating the need for high-energy ball milling and reducing overall energy consumption while being environmentally friendly.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent replaces mechanical mixing and high-energy ball milling processes with a chemical solution-based spray pyrolysis method. The precursor solution is atomized into droplets and converted to particles through flame pyrolysis, substituting mechanical energy-intensive processes with a chemical transformation approach that is both energy-efficient and environmentally benign.

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

2Manufacturing precision

If conventional methods are used to produce solid electrolyte particles, then the particle size distribution is non-uniform, but the particles can still be used for thin film fabrication

Engineering Contradiction:
Improveparticle size uniformityVSAvoidmanufacturing complexity
Core Design Contradiction:
Manufacturing precisionVSEase of manufacture

Solution Approach 1:

The patent segments the particle formation process into controlled stages: (1) dissolution of precursors in organic solvents to form a homogeneous solution, (2) atomization of the solution into fine droplets, and (3) pyrolytic conversion to uniform particles. This segmentation allows precise control over particle size distribution (20 nm to 10 μm) and eliminates the need for post-synthesis size control methods.

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The patent performs preliminary action by preparing a homogeneous precursor solution before particle formation. The inorganic precursors (lithium nitrate, lanthanum nitrate, zirconium nitrate) are thoroughly dissolved in organic solvents like ethanol or methanol, ensuring uniform distribution of all elements before pyrolysis. This preliminary homogenization guarantees uniform particle composition and size distribution in the final product.

Inventive Principle:
Principle #10Preliminary action

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 produces high-quality, uniform c-LLZO particles and films with improved ionic conductivity, enabling safer and more efficient lithium-based batteries suitable for industrial scale-up.

Implementation Method 1

converting the aerosol to solid powders at elevated temperature

Methodology Applied
Scientific EffectPyrolysis: Pyrolysis

Implementation Method 2

generating an aerosol of said solution; converting the aerosol to solid powders

Methodology Applied
Scientific EffectEvaporation: Evaporation

Implementation Method 3

annealing said solid powders to provide the solid electrolyte particles

Methodology Applied
Scientific EffectAnnealing: Annealing

Data Source

PatentUS12463248B2Environmentally preferable method of making solid electrolyte and integration of metal anodes thereof
Publication Date: 2025.11.04 SHENZHEN INX ENERGY TECHNOLOGY CO LTD
  • US12463248B2 patent drawing
  • US12463248B2 patent drawing
  • US12463248B2 patent drawing

AI summary

A method of pairing a cubic Li7La3Zr2O12 (c-LLZO) based solid-state electrolyte film/membrane and lithium metal, with a metal oxide interface between the film/membrane and lithium metal, wherein the metal oxide is La2O3, CuO, ZrO2, HfO2, or any combination thereof. A method of pairing a c-LLZO based solid-state electrolyte film/membrane and lithium metal comprises treating the film/membrane with a gas plasma before applying metal lithium. An integrated combination of a solid-state electrolyte and a metal anode comprises a c-LLZO based solid-state electrolyte film/membrane with a thickness of about 5-50 μm, a metal anode integrated on the solid-state electrolyte film/membrane, and a metal oxide interface between the film/membrane and lithium metal, wherein the metal oxide is La2O3, CuO, ZrO2, HfO2, or any combination thereof, and the metal anode is lithium metal with a thickness of 5-50 μm.