Sulfur Cathode Composition With In-Situ Li3PS4 for High-Loading Li-S Batteries

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Solution Overview

Problem

Existing all-solid-state lithium-sulfur batteries suffer from poor ionic conductivity and low specific capacity, particularly at high loading levels, due to the low participation of active materials in the charge-discharge cycle.

Innovation Solution

A cathode material comprising porous carbon conductive agents, additives (phosphorus pentasulfide or phosphorus trisulfide), and a solid electrolyte (lithium phosphorus sulfur chloride) is prepared through a multi-step ball milling and sintering process, forming a lithium phosphorus sulfur (Li3PS4) solid electrolyte that enhances ionic conductivity and active material utilization.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If traditional complex materials and processes are used for all-solid-state Li-S battery cathode systems, then the battery structure can be formed, but the performance is poor at high loading levels and cycling stability is insufficient

Engineering Contradiction:
Improvecycling stabilityVSAvoidmaterials and processes complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The patent uses a composite cathode material system consisting of sulfur active material, lithium phosphorus sulfur solid electrolyte, and conductive carbon. This composite structure combines the high capacity of sulfur with the ionic conductivity of Li3PS4 and the electrical conductivity of carbon, achieving both high performance and cycling stability without requiring overly complex preparation processes

Inventive Principle:
Principle #40Composite materials

Solution Approach 2:

The patent optimizes the composition ratios of the cathode materials, specifically controlling the content of sulfur (38-44 parts), solid electrolyte (32-40 parts), and conductive carbon (10 parts). By adjusting these parameters within optimal ranges, the battery achieves high specific capacity and cycling stability at high loading levels

Inventive Principle:
Principle #35Parameter changes

2Quantity of substance

If sulfur is used as the active material with high theoretical capacity, then specific capacity can be maximized, but ionic conductivity remains poor limiting actual performance

Engineering Contradiction:
Improvespecific capacityVSAvoidionic conductivity
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The patent introduces lithium phosphorus sulfur (Li3PS4) solid electrolyte as an intermediary substance between sulfur and the electrolyte. This intermediary layer provides excellent ionic conductivity while allowing sulfur to fully participate in charge-discharge reactions, thus simultaneously achieving high specific capacity and good ionic conductivity

Inventive Principle:
Principle #24Intermediary (Mediator)

Solution Approach 2:

The cathode is designed as a composite material system where sulfur (providing high capacity) is combined with Li3PS4 solid electrolyte (providing ionic conductivity) and conductive carbon (providing electrical conductivity). This composite structure allows the advantages of each component to complement each other, resolving the contradiction between capacity and conductivity

Inventive Principle:
Principle #40Composite materials

3Quantity of substance

If high areal loading is applied to increase energy density, then battery capacity increases, but active material participation in charge-discharge cycle decreases

Engineering Contradiction:
Improveareal loadingVSAvoidactive material utilization
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The patent creates a local conductive network structure where Li3PS4 solid electrolyte forms ionic conduction channels throughout the cathode. This local optimization of ionic conductivity ensures that even at high areal loading, lithium ions can efficiently reach and react with sulfur particles throughout the entire cathode structure, maintaining high active material utilization

Inventive Principle:
Principle #3Local quality

Solution Approach 2:

The Li3PS4 solid electrolyte acts as a mediator that facilitates lithium ion transport from the bulk electrolyte to the sulfur active material throughout the cathode. This intermediary function ensures uniform lithium ion distribution and reaction throughout the cathode, preventing poor utilization at high loading levels

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 cathode material improves the specific capacity and cycling stability of lithium-sulfur batteries under high areal loading by facilitating faster lithium ion conduction and full participation of active materials in the charge-discharge cycle.

Implementation Method 1

elemental sulfur reacts with lithium ions during battery discharge to form lithium sulfide, which can react with the additive to in-situ generate a lithium phosphorus sulfur (Li 3 PS 4) solid electrolyte

Methodology Applied
Scientific EffectChemical reaction: Chemical Bonding

Implementation Method 2

forms an ionic conductive network, allowing lithium ions to conduct faster

Methodology Applied
Scientific EffectIonic conduction: Conduction (electrical)

Implementation Method 3

facilitates better attachment of phosphorus pentasulfide to the surface and better penetration of active materials into the pores

Methodology Applied
Scientific EffectAdsorption: Adsorption

Implementation Method 4

better penetration of active materials into the pores

Methodology Applied
Scientific EffectDiffusion: Diffusion

Data Source

PatentEP4708373A1Positive electrode material and preparation method therefor, positive electrode sheet, and lithium-sulfur battery
Publication Date: 2026.03.11 TSINGHUA UNIVERSITY
  • EP4708373A1 patent drawingFigure 1
  • EP4708373A1 patent drawingFigure 2
  • EP4708373A1 patent drawingFigure 3

AI summary

The present application provides a cathode material comprising the following raw materials in parts by weight: 10 parts of a porous carbon conductive agent, 7 to 14 parts of an additive, 38 to 44 parts of an active material, and 32 to 40 parts of a solid electrolyte, wherein the active material comprises sulfur powder, and the additive comprises one or both of phosphorus pentasulfide and phosphorus trisulfide. Elemental sulfur reacts with lithium ions during battery discharge to form lithium sulfide, which can react with the additive to in-situ generate a lithium phosphorus sulfur solid electrolyte. The lithium phosphorus sulfur solid electrolyte not only enables most of the active material to participate in the charge-discharge cycle, improving the utilization rate of the active material, but also forms an ionic conductive network, allowing lithium ions to conduct faster. It also enhances the ionic conductivity of the cathode material, achieving high specific capacity and cycling stability in all-solid-state lithium-sulfur batteries under high areal loading conditions.