Lithium Argryrodite Solid Electrolyte Phase Purity

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Solution Overview

Problem

The production of phase-pure lithium-rich solid-state compounds, particularly lithium argyrodites, is challenging due to their sensitivity to starting materials and crucible materials, leading to the formation of by-products and limited lithium ion mobility, which affects their use as solid electrolytes in electrochemical energy storage.

Innovation Solution

Development of lithium argyrodites with the general formula Li_(10-n-x)B_n+X_2-xY_x, where B_n+ includes elements like P, As, Ge, and Ga, X_2- includes S, Se, and Y includes Cl, Br, and I, allowing for phase-pure production and high lithium ion mobility, usable as solid electrolytes over a wide temperature range.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Manufacturing precision

If conventional production methods are used for lithium-rich solid-state compounds, then production can proceed with standard materials, but phase purity is compromised and by-products form due to sensitivity to starting materials and crucible materials

Engineering Contradiction:
Improvephase purityVSAvoidby-product formation
Core Design Contradiction:
Manufacturing precisionVSObject-generated harmful factors

Solution Approach 1:

The patent employs an intermediary substance (iodine or bromine) during the synthesis process that mediates the reaction between lithium sulfide and phosphorus pentasulfide. This intermediary enables phase-pure formation of Li6PS5X compounds by controlling the reaction pathway and preventing unwanted by-products, thereby resolving the contradiction between standard production methods and phase purity requirements.

Inventive Principle:
Principle #24Intermediary (Mediator)

2Temperature

If standard solid electrolyte materials are used, then electrochemical energy storage can be implemented, but temperature sensitivity limits the operational temperature range

Engineering Contradiction:
Improveoperational temperature rangeVSAvoidtemperature sensitivity
Core Design Contradiction:
TemperatureVSReliability

Solution Approach 1:

The patent applies parameter changes by modifying the chemical composition of the solid electrolyte through substitution of halogen atoms (Cl, Br, I) at the X position in the Li6PS5X formula. This compositional parameter change fundamentally alters the material's thermal properties, enabling stable operation across an extended temperature range from -150°C to 600°C and reducing temperature sensitivity.

Inventive Principle:
Principle #35Parameter changes

3Speed

If conventional lithium electrolytes are used, then electrochemical energy storage is achievable, but lithium ion mobility is limited affecting performance

Engineering Contradiction:
Improvelithium ion mobilityVSAvoidion conductivity
Core Design Contradiction:
SpeedVSReliability

Solution Approach 1:

The patent utilizes composite material design by creating Li6PS5X compounds that combine lithium sulfide, phosphorus sulfide, and halogen components in a specific crystalline structure. This composite approach optimizes the material's ionic conductivity and lithium ion mobility while maintaining structural stability, thereby improving both speed and reliability of ion transport.

Inventive Principle:
Principle #40Composite materials

Data Source

PatentEP2197795B1Lithium argyrodite
Publication Date: 2013.01.02 UNIVERSITY OF SIEGEN

AI summary

The invention relates to lithium argyrodite of the general formula (I): Li+ (12-n-x)Bn+ X2- 6-x Y- x (I), where Bn+ is selected from the group P, As, Ge, Ga, Sb, Si, Sn, Al, In, Ti, V, Nb, and Ta, X2 - is selected from the group S, Se, and Te, Y- is selected from the group Cl, Br, I, F, CN, OCN, SCN, N3, and where 0 = x = 2, and a method for the production thereof, and the use thereof as a lithium-ion electrolyte in primary and secondary electrochemical energy storage.