Argyrodite Solid Electrolyte Synthesis via Solvent Exchange

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Solution Overview

Problem

Current methods for producing solid-state argyrodite electrolytes are inefficient, as they often result in low-phase-purity products with non-uniform stoichiometry and are time-consuming, making them unsuitable for scalable manufacturing.

Innovation Solution

A method involving the formation of a precursor by mixing a suspension of Li3PS4 with a solution containing Li2S and LiX in ester and alcohol solvents, followed by solvent removal to produce a solid-state argyrodite electrolyte with improved ionic conductivity, represented by the formula Li6PS5X, where X is chloride, bromide, or iodine.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Manufacturing precision

If ball-milling methods are used to prepare solid-state argyrodite electrolytes, then the manufacturing process is simple, but the product has low phase purity, non-uniform stoichiometry, and poor scalability

Engineering Contradiction:

Improvephase purity and stoichiometry uniformityVSAvoidmanufacturing scalability and time efficiency

Core Design Contradiction:

Manufacturing precisionVSProductivity

Solution Approach 1:

The patent changes the fundamental parameters of the preparation method by transitioning from mechanical ball-milling to a chemical solution-based approach. The new method uses specific solvent systems (esters and alcohols) and controlled chemical reactions to achieve uniform stoichiometry and high phase purity, directly resolving the contradiction between manufacturing precision and productivity

Inventive Principle:

Principle #35Parameter changes

Solution Approach 2:

The patent replaces the mechanical ball-milling system with a chemical solution-based system. Instead of using mechanical force to mix and react powders, the invention uses chemical dissolution and precipitation mechanisms in ester-alcohol solvent systems, which enables better control over phase purity and stoichiometry while improving scalability

Inventive Principle:

Principle #28Mechanics substitution (Replace mechanical system)

2Loss of time

If ball-milling methods are used to prepare solid-state argyrodite electrolytes, then the process can be implemented with simple equipment, but the process is time-consuming and energy-consuming

Engineering Contradiction:

Improvepreparation timeVSAvoidenergy consumption

Core Design Contradiction:

Loss of timeVSUse of energy by moving object

Solution Approach 1:

The patent changes the time and energy parameters by using a chemical solution method that proceeds at ambient or mild temperatures without requiring prolonged mechanical processing. The chemical reaction in solution occurs much faster than mechanical ball-milling, significantly reducing both preparation time and energy consumption while maintaining simple equipment requirements

Inventive Principle:

Principle #35Parameter changes

3Reliability

If conventional methods are used to prepare solid-state argyrodite electrolytes, then the process is easy to implement, but the ionic conductivity is insufficient

Engineering Contradiction:

Improveionic conductivityVSAvoidmanufacturing process simplicity

Core Design Contradiction:

ReliabilityVSEase of manufacture

Solution Approach 1:

The patent employs a composite solvent system combining esters and alcohols, which creates optimal conditions for the chemical reaction and product formation. This composite approach enhances ionic conductivity by ensuring uniform stoichiometry and phase purity, while the process remains simple to implement using standard laboratory equipment

Inventive Principle:

Principle #40Composite materials

Solution Approach 2:

The ester-alcohol solvent system acts as an intermediary medium that facilitates the chemical reaction between reactants. The solvents dissolve reactants uniformly, control reaction kinetics, and enable precise stoichiometry control, thereby achieving high ionic conductivity without complicating the manufacturing process

Inventive Principle:

Principle #24Intermediary (Mediator)

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 solid-state argyrodite electrolytes with ionic conductivity ranging from 1.0×10−4 to 10×10−3 S/cm at 25°C, enhancing the manufacturing process and achieving high-phase-purity products with improved scalability.

Implementation Method 1

contacting a first suspension and a first solution to form a precursor, where the first suspension includes Li3PS4 and an ester solvent, and the first solution includes Li2S, LiX, and an alcohol solvent

Methodology Applied

Scientific EffectSolvation: Solvation

Implementation Method 2

removing the ester solvent and the alcohol solvent from the precursor to form the solid-state argyrodite electrolyte

Methodology Applied

Scientific EffectEvaporation: Evaporation

Data Source

PatentUS20230024667A1Argyrodite solid electrolytes for solid-state batteries and methods of making the same

Publication Date: 2023.01.26 GM GLOBAL TECHNOLOGY OPERATIONS LLC

AI summary

The present disclosure provides a method for making a solid-state argyrodite electrolyte represented by Li6PS5X (where X is selected from chloride, bromide, iodine, or a combination thereof) having an ionic conductivity greater than or equal to about 1.0×10−4 S/cm to less than or equal to about 10×10−3 S/cm at about 25° C. The method may include contacting a first suspension and a first solution to form a precursor, where the first suspension is a Li3PS4 suspension including an ester solvent and the first solution is a Li2S and LiX (where X is selected from chloride, bromide, or iodine, or a combination thereof) solution including an alcohol solvent; and removing the ester solvent and the alcohol solvent from the precursor to form the solid-state argyrodite electrolyte.