Ionically Conductive Films With Plasma-Formed Amorphous Electrolytes

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Solution Overview

Problem

Current methods for producing solid-state batteries face challenges in achieving high ionic conductivity while maintaining amorphous structures with higher alkali metal content, particularly in glassy electrolytes like LIPON, and require versatile methods to control various compositions and structures such as amorphous, crystalline, and glass-ceramic forms.

Innovation Solution

The development of ionically conductive compositions containing alkali or alkaline earth metals with specific elements like silicon, phosphorus, and nitrogen, produced through inductive plasma processing, which allows for the creation of high-lithium content oxynitride glasses with high ionic conductivity and the ability to form films or membranes with controlled crystallinity and amorphous character.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If conventional glass making processes are used to produce glassy LIPON electrolytes, then the manufacturing process is simple and well-established, but the ionic conductivity remains low and Li content must be kept low to maintain amorphous structure

Engineering Contradiction:
Improveionic conductivityVSAvoidmanufacturing complexity
Core Design Contradiction:
ReliabilityVSEase of manufacture

Solution Approach 1:

The patent changes the manufacturing parameters by using plasma processing instead of conventional glass making, enabling higher Li and N content while maintaining amorphous structure. The plasma process parameters (power, gas flow, temperature) are optimized to achieve the desired compositional range and structural properties that conventional methods cannot attain.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent replaces the thermal-mechanical conventional glass making process with a plasma-based process. The plasma provides energetic particles and excited states that enable different reaction pathways and kinetics, allowing incorporation of higher Li and N content while maintaining amorphous structure, thus resolving the contradiction between ionic conductivity and manufacturing simplicity.

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

2Reliability

If Li and N content are increased to improve ionic conductivity in glassy electrolytes, then ionic conductivity improves, but maintaining amorphous structure becomes difficult and crystallization occurs

Engineering Contradiction:
Improveionic conductivityVSAvoidamorphous structure stability
Core Design Contradiction:
ReliabilityVSStability of the object's composition

Solution Approach 1:

The plasma processing parameters are specifically optimized to achieve rapid cooling rates and controlled energy input that prevent crystallization even at high Li and N content. The plasma provides sufficient energy for atomic rearrangement during processing but rapid quenching prevents ordered crystal formation, thus maintaining amorphous structure while achieving high ionic conductivity.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent uses composite oxide-nitride-glass compositions where multiple components work synergistically. The specific combination of metal oxides with nitrogen and glass formers creates a composition that favors amorphous structure formation while providing high ionic conductivity pathways, resolving the contradiction between composition and structural stability.

Inventive Principle:
Principle #40Composite materials

3Reliability

If Si is introduced into glassy electrolyte to improve ionic conductivity and maintain amorphous structure with higher Li content, then ionic conductivity improves and amorphous structure is easier to maintain, but the composition becomes more complex

Engineering Contradiction:
Improveionic conductivityVSAvoidcomposition complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The patent deliberately creates composite oxide-nitride-glass materials with Si as a key component. The Si-based glass network provides structural stability and facilitates amorphous phase formation, while the composite nature allows tuning of ionic conductivity through controlled composition ratios. The complexity is managed through systematic composition design rather than random addition of components.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

Si serves multiple functions in the composition: it acts as a glass former to stabilize amorphous structure, provides pathways for ionic conduction, and enables higher Li content incorporation. This multi-functionality reduces the need for additional components, managing overall composition complexity while achieving multiple performance goals simultaneously.

Inventive Principle:
Principle #6Universality (Multi-functionality)

4Ease of manufacture

If standard ceramic powder processing is used for crystalline electrolytes, then the manufacturing process is well-established, but a significant amount of excess Li is required to achieve correct compositions and structures

Engineering Contradiction:
Improvemanufacturing process maturityVSAvoidexcess Li requirement
Core Design Contradiction:
Ease of manufactureVSLoss of substance

Solution Approach 1:

The patent replaces standard ceramic powder processing with plasma processing. The plasma enables direct synthesis of crystalline electrolytes with precise stoichiometry control, eliminating the need for excess Li that is typically required in conventional ceramic processing to compensate for losses during sintering and to ensure complete reaction. The plasma's high energy density and controlled atmosphere prevent material loss.

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

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 enables the production of solid electrolytes with enhanced ionic conductivity, reduced sintering temperatures, and cost-effective membrane processing, suitable for advanced manufacturing techniques like additive manufacturing, and achieves ionic conductivities comparable to commercial powders.

Implementation Method 1

subjecting a precursor material to a thermal process in which the precursor material is at least partially vaporized

Methodology Applied
Scientific EffectVaporization: Evaporation

Implementation Method 2

subsequently cooled (quenched, i.e., condensed) on a substrate to form the ionically conductive continuous film

Methodology Applied
Scientific EffectCondensation: Condensation

Implementation Method 3

The plasma process, and more specifically, an inductively coupled plasma (ICP) process

Methodology Applied
Scientific EffectInductive heating: Induction Heating

Data Source

PatentUS11807543B2Ionically conductive powders and films, and methods of preparation
Publication Date: 2023.11.07 UT BATTELLE LLC
  • US11807543B2 patent drawing
  • US11807543B2 patent drawing
  • US11807543B2 patent drawing

AI summary

A solid ionically conductive composition (e.g., nanoparticles of less than 1 micron or a continuous film) comprising at least one element selected from alkali metal, alkaline earth metal, aluminum, zinc, copper, and silver in combination with at least two elements selected from oxygen, sulfur, silicon, phosphorus, nitrogen, boron, gallium, indium, tin, germanium, arsenic, antimony, bismuth, transition metals, and lanthanides. Also described is a battery comprising an anode, a cathode, and a solid electrolyte (corresponding to the above ionically conductive composition) in contact with or as part of the anode and/or cathode. Further described is a thermal (e.g., plasma-based) method of producing the ionically conductive composition. Further described is a method for using an additive manufacturing (AM) process to produce an object constructed of the ionically conductive composition by use of particles of the ionically conductive composition as a feed material in the AM process.