Li2S Composite Cathode Using Halogenated LPS for Solid-State Cycling

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Solution Overview

Problem

Current all solid-state lithium secondary batteries face challenges in achieving sufficient lithium ion diffusivity, mechanical stability, and preventing polysulfide dissolution, which leads to degradation and reduced performance.

Innovation Solution

A composite cathode material is developed through a single-step ball-milling process combining Li2S, halogenated lithium phosphorous sulfide (LPS-X) particles, and carbon, which results in a highly reversible and conductive cathode with enhanced electrochemical properties, utilizing sulfide solid electrolytes as both ionic conductors and redox mediators.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If solid electrolyte material is used in all solid-state batteries, then safety and stability are improved, but lithium ion diffusivity is insufficient

Engineering Contradiction:
Improvesafety and stabilityVSAvoidlithium ion diffusivity
Core Design Contradiction:
ReliabilityVSSpeed

Solution Approach 1:

The patent uses a composite solid electrolyte system combining sulfide-based solid electrolyte particles with a conductive matrix material. This composite structure allows the sulfide particles to provide high lithium ion conductivity and stability, while the conductive matrix ensures sufficient lithium ion diffusivity throughout the electrode, resolving the contradiction between safety/stability and ion transport speed.

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent employs a porous electrode structure where sulfide solid electrolyte particles are distributed within a conductive matrix. The porous architecture provides pathways for lithium ion diffusion while maintaining intimate contact between active material, solid electrolyte, and conductive matrix, ensuring both high safety/stability and adequate ion diffusivity.

Inventive Principle:
Principle #31Porous materials

2Quantity of substance

If electrode components undergo volume changes during charging and discharging, then electrochemical capacity is improved, but mechanical stress and loss of contact occur

Engineering Contradiction:
Improveelectrochemical capacityVSAvoidmechanical stability
Core Design Contradiction:
Quantity of substanceVSStrength

Solution Approach 1:

The patent uses a flexible conductive matrix that can accommodate volume changes of electrode components during charging and discharging. This matrix acts as a buffer that maintains mechanical integrity and prevents loss of contact between components, allowing the electrode to achieve high electrochemical capacity without suffering from mechanical stress or contact degradation.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The composite electrode structure consisting of active material particles, solid electrolyte particles, and conductive matrix provides mechanical flexibility. The conductive matrix serves as a resilient framework that absorbs volume expansion and contraction, maintaining electrical and ionic connectivity throughout cycling, thus enabling high capacity with good mechanical stability.

Inventive Principle:
Principle #40Composite materials

3Quantity of substance

If sulfur active material is used in lithium-sulfur batteries, then theoretical capacity and energy density are improved, but polysulfide dissolution and degradation occur

Engineering Contradiction:
Improvetheoretical capacity and energy densityVSAvoidcycling stability
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The patent extracts sulfur from the traditional liquid electrolyte environment and confines it within a solid-state matrix. By using sulfide solid electrolyte particles embedded in a conductive matrix, the system eliminates polysulfide dissolution while maintaining high sulfur utilization, achieving both high capacity and cycling stability.

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The conductive matrix acts as an intermediary between sulfur active material and the external circuit. It provides a stable solid-state environment that prevents polysulfide formation and dissolution, while still enabling efficient electron and ion transport, thus preserving both high capacity and cycling reliability.

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 composite cathode achieves high areal capacities and cycling stability, with 90% retention after 500 cycles, and maintains stability without liquid electrolytes, while the ball-milling process enhances lithium ion transport and electrochemical kinetics.

Implementation Method 1

ball-milling the mixture in the ball-milling container to provide a ball-milled composite material such that at least part of the LPS-X compound contained in at least part of the LPS-X particles is converted to the LPS compound

Methodology Applied
Scientific EffectMechanical energy conversion: Mechanical Force

Implementation Method 2

utilizing sulfide solid electrolytes as both ionic conductors and redox mediators

Methodology Applied
Scientific EffectIonic conduction: Conduction (electrical)

Implementation Method 3

utilizing sulfide solid electrolytes as both ionic conductors and redox mediators

Methodology Applied
Scientific EffectRedox reactions: Redox Reactions

Data Source

PatentUS20250266450A1Electrode composite materials, electrodes comprising same, and all solid state batteries comprising same, and methods of making same
Publication Date: 2025.08.21 LG ENERGY SOLUTION LTD
  • US20250266450A1 patent drawing
  • US20250266450A1 patent drawing
  • US20250266450A1 patent drawing

AI summary

An electrode composite material and a method of making same are disclosed. A mixture that includes lithium sulfide (Li2S) particles containing a Li2S compound, carbon particles, and halogenated lithium phosphorous sulfide (LPS-X) particles containing an LPS-X (X is F, Cl, Br, and/or I) compound are provided. The LPS-X particles have crystallinity which can be confirmed with XRD of the LPS-X particles or the mixture showing XRD peaks indicative of crystalline LPS-X. The mixture does not include lithium phosphorous sulfide (LPS) particles made of an LPS compound. The mixture is ball-milled to provide a ball-milled composite material. At least part of the LPS-X compound contained in at least part of the LPS-X particles is converted to the LPS compound. XRD of the ball-milled composite material shows none of the XRD peaks indicative of crystalline LPS-X.