Coated Silicon Anode Material for Swelling-Resistant Li-Ion Batteries

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Solution Overview

Problem

Silicon-based negative electrode active materials in lithium secondary batteries face issues with volumetric swelling during lithium intercalation, leading to degradation of charge/discharge cycle life due to cracking and mis-contact with the current collector.

Innovation Solution

A negative electrode active material comprising silicon particles with a full width at half maximum (FWHM) of 2-10 in the particle diameter distribution and a coating layer of carbon and/or polymer, which prevents pulverization and side reactions, enhancing conductivity and reaction reversibility.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If Si-based materials are used as negative electrode active materials to achieve high theoretical capacity, then capacity is improved, but volumetric swelling occurs during lithium intercalation leading to cracking and degradation of charge/discharge cycle life

Engineering Contradiction:
ImprovecapacityVSAvoidcharge/discharge cycle life
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The patent divides the negative electrode into multiple layers: a first negative electrode layer containing Si-based active material and a second negative electrode layer containing carbonaceous material. This segmentation isolates the high-capacity Si-based material from direct contact with electrolyte while maintaining its capacity benefits, and the carbonaceous layer provides structural stability to prevent swelling-induced cracking, thus resolving the contradiction between high capacity and cycle life reliability

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The patent creates a composite negative electrode structure combining Si-based active material with carbonaceous material in specific weight ratios (Si-based: 30-80 wt%, carbonaceous: 20-70 wt%). This composite approach allows the Si-based material to provide high theoretical capacity while the carbonaceous material provides structural integrity and swelling resistance, simultaneously achieving both high capacity and improved charge/discharge cycle life

Inventive Principle:
Principle #40Composite materials

2Quantity of substance

If Si-based materials are used to achieve high theoretical capacity, then capacity is improved, but cracking occurs due to volumetric swelling causing mis-contact between active material and current collector

Engineering Contradiction:
ImprovecapacityVSAvoidstructural integrity
Core Design Contradiction:
Quantity of substanceVSStrength

Solution Approach 1:

The patent separates the Si-based active material into a distinct first negative electrode layer and provides a second negative electrode layer with carbonaceous material. This segmentation prevents the Si-based material from undergoing free volumetric swelling that causes cracking, while maintaining its high capacity properties through controlled structural configuration

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The patent forms a composite structure where Si-based material (30-80 wt%) is combined with carbonaceous material (20-70 wt%). The carbonaceous component acts as a structural framework that constrains volumetric swelling of the Si-based material during lithium intercalation, preventing cracking and maintaining structural integrity while preserving high capacity

Inventive Principle:
Principle #40Composite materials

3Reliability

If carbonaceous materials are used as negative electrode active materials to achieve high stability and reversibility, then reliability is improved, but capacity is limited

Engineering Contradiction:
Improvestability and reversibilityVSAvoidcapacity
Core Design Contradiction:
ReliabilityVSQuantity of substance

Solution Approach 1:

The patent assigns multiple functions to different layers: the first negative electrode layer with Si-based material provides high capacity function, while the second negative electrode layer with carbonaceous material provides stability and reversibility function. This multi-functional assignment allows the overall electrode to achieve both high capacity and high reliability simultaneously

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

Solution Approach 2:

The patent creates a composite negative electrode where Si-based material (30-80 wt%) contributes high theoretical capacity and carbonaceous material (20-70 wt%) contributes high stability and reversibility. The synergistic combination allows the electrode to achieve capacity values exceeding traditional carbonaceous materials while maintaining their stability and reversibility characteristics

Inventive Principle:
Principle #40Composite materials

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 solution significantly improves both life and output characteristics of lithium secondary batteries by preventing particle pulverization and maintaining physical binding, thus extending cycle life and ensuring high capacity retention.

Implementation Method 1

a coating layer surrounding the silicon particles, wherein the silicon particles have a full width at half maximum (FWHM) of peak ranging from 2 to 10 in the particle diameter distribution having an average particle diameter (D 50 ) of 1-30 μm, and the coating layer includes at least one of carbon and a polymer

Methodology Applied
Scientific EffectMechanical stress absorption:

Implementation Method 2

the coating layer includes at least one of carbon and a polymer

Methodology Applied
Scientific EffectPhysical barrier formation:

Implementation Method 3

the coating layer includes at least one of carbon and a polymer

Methodology Applied
Scientific EffectElectrical conduction: Conduction (electrical)

Implementation Method 4

Si-based negative electrode active materials are problematic in that they undergo a change in crystal structure during lithium intercalation and storage to cause volumetric swelling

Methodology Applied
Scientific EffectVolumetric swelling: Thermal Expansion

Implementation Method 5

the silicon particles have a full width at half maximum (FWHM) of peak ranging from 2 to 10 in the particle diameter distribution having an average particle diameter (D 50 ) of 1-30 μm

Methodology Applied
Scientific EffectParticle size distribution control:

Data Source

PatentEP3846257B1Negative electrode active material for lithium secondary battery, and negative electrode and lithium secondary battery including the same
Publication Date: 2024.07.24 LG ENERGY SOLUTION LTD
  • EP3846257B1 patent drawingFigure 1~2
  • EP3846257B1 patent drawingFigure 3~4

AI summary

Disclosed is a negative electrode active material for a lithium secondary battery which includes: silicon particles; and a coating layer surrounding the silicon particles, wherein the silicon particles have a full width at half maximum (FWHM) of peak ranging from 2 to 10 in the particle diameter distribution having an average particle diameter (D50) of 1-30 µm, and the coating layer includes at least one of carbon and a polymer. A negative electrode and lithium secondary battery including the negative electrode active material are also disclosed.