Tri-Layer Silicon-Graphite Negative Electrode for Lithium Battery

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Solution Overview

Problem

Lithium secondary batteries face issues with non-uniform swelling and separation of electrodes due to the volumetric changes of silicon-based negative electrode active materials, leading to performance degradation and safety concerns.

Innovation Solution

A tri-layer structure for the negative electrode is introduced, comprising a silicon-based active material layer sandwiched between two layers of carbonaceous active materials with different shapes and surface treatments, enhancing adhesion and conductivity to prevent swelling and improve electrical characteristics.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon-based negative electrode active material is used to increase lithium capacity, then energy density is improved, but volume expansion during charge/discharge causes electrode separation and performance degradation

Engineering Contradiction:
Improvelithium capacityVSAvoidelectrode structure stability
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

The negative electrode is divided into multiple layers: a first carbonaceous layer directly on the current collector, a silicon-based active material layer in the middle, and a second carbonaceous layer on top. This segmentation isolates the silicon layer's volume expansion from the current collector and outer electrode surface, preventing electrode separation while maintaining high lithium capacity.

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The negative electrode uses a composite structure combining carbonaceous materials (graphite or hard carbon) with silicon-based active material. The carbonaceous layers provide structural stability and accommodate volume changes, while the silicon layer provides high lithium capacity, creating a composite that balances both requirements.

Inventive Principle:
Principle #40Composite materials

2Quantity of substance

If silicon-based negative electrode active material is used to increase lithium capacity, then energy density is improved, but contact resistance between particles increases due to volume expansion

Engineering Contradiction:
Improvelithium capacityVSAvoidelectrical conductivity
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

The silicon-based active material layer is segmented and surrounded by conductive carbonaceous materials on both sides. This segmentation ensures that even when silicon particles expand, they remain in electrical contact with the conductive carbon network, maintaining reliable electron transport pathways.

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The carbonaceous materials act as intermediary conductive phases between the silicon particles and the current collector. These intermediaries maintain electrical contact during volume expansion, preventing increase in contact resistance while allowing the silicon to undergo lithiation/delithiation.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Reliability

If graphite-based particles are used to surround silicon negative electrode active material to improve conductivity, then electrical conductivity is improved, but contact between graphite particles and silicon particles degrades due to volume expansion

Engineering Contradiction:
Improveelectrical conductivityVSAvoidparticle contact stability
Core Design Contradiction:
ReliabilityVSStability of the object's composition

Solution Approach 1:

The carbonaceous particles (graphite or hard carbon) form flexible surrounding layers that can accommodate the volume expansion of silicon particles during lithiation. These flexible carbon shells maintain contact with the silicon particles throughout the charge/discharge cycles, preserving both conductivity and contact stability.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

The negative electrode creates a composite structure where carbonaceous materials and silicon-based active material are intimately mixed and coated together. This composite approach ensures that the carbon particles remain in stable contact with silicon particles even during volume expansion, maintaining both conductivity and structural integrity.

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 tri-layer structure effectively inhibits non-uniform swelling and separation, enhancing the adhesion between the electrode and current collector, and significantly improving output and life characteristics of the battery.

Implementation Method 1

the first carbonaceous negative electrode active material includes spherical shaped particles, which spherical shaped particles having a sphericity of 0.90-0.99, said spherical shaped particles including an oxidized surface portion

Methodology Applied
Scientific EffectOxidation: Oxidation

Implementation Method 2

said spherical shaped particles including an oxidized surface portion and/or carbon-coated surface portion, and the second carbonaceous negative electrode active material includes flake shaped particles having a sphericity of 0.70-0.89, said flake shaped particles including a carbon-coated surface portion

Methodology Applied
Scientific EffectCarbon coating: Coatings

Implementation Method 3

various types of carbonaceous materials capable of lithium intercalation/deintercalation

Methodology Applied
Scientific EffectIntercalation: Absorption (physical)

Implementation Method 4

various types of carbonaceous materials capable of lithium intercalation/deintercalation

Methodology Applied
Scientific EffectDeintercalation: Desorption

Data Source

PatentUS11283062B2Negative electrode for lithium secondary battery and lithium secondary battery comprising same
Publication Date: 2022.03.22 LG ENERGY SOLUTION LTD
  • US11283062B2 patent drawing
  • US11283062B2 patent drawing

AI summary

A negative electrode for a lithium secondary battery (and a lithium secondary battery including the same) including: a negative electrode current collector; a first negative electrode mixture layer present on at least one surface of the negative electrode current collector and including a first carbonaceous negative electrode active material, a first polymer binder and a first conductive material; a second negative electrode mixture layer present on a top surface of the first negative electrode mixture layer and including a silicon-based negative electrode active material, a second polymer binder and a second conductive material; and a third negative electrode mixture layer present on a top surface of the second negative electrode mixture layer and including a second carbonaceous negative electrode active material, a third polymer binder and a third conductive material.