Pre-Lithiated Oxide Coating for Silicon Anode Volume Expansion

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Solution Overview

Problem

Lithium secondary batteries using silicon-based negative electrodes face issues with rapid volume expansion and unstable solid electrolyte interface (SEI) formation, leading to capacity fading and reduced cycle life due to lithium ion trapping and irreversible reactions.

Innovation Solution

A multi-layer composite structure is developed with a pre-lithiated metal oxide as the outermost shell, comprising a silicon-based negative electrode core, a conductive carbon material inner shell, and a pre-lithiated metal oxide outer shell, formed through a lithiation reaction, to stabilize the SEI and reduce lithium ion trapping.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon-based materials are used as negative electrode material, then high theoretical capacity is achieved, but rapid volume expansion occurs during charging and discharging

Engineering Contradiction:
Improvetheoretical capacityVSAvoidstructural stability
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

The patent employs a multi-layer nested structure where the silicon-based negative electrode particle is sequentially coated with conductive carbon material and then pre-lithiated metal oxide. This nested configuration allows the silicon core to maintain its high capacity function while being progressively protected by outer layers that constrain volume expansion and stabilize the structure during lithium ion insertion and extraction cycles.

Inventive Principle:
Principle #7Nested doll (Nesting)

Solution Approach 2:

The patent creates a composite material system combining silicon-based materials with conductive carbon and pre-lithiated metal oxide. This composite structure integrates the high capacity advantage of silicon with the structural stability and protective properties of the coating materials, achieving both high theoretical capacity and resistance to volume expansion through material composition rather than relying on a single material's properties.

Inventive Principle:
Principle #40Composite materials

2Stability of the object's composition

If silicon oxide is used as negative electrode material, then structural stability is improved, but unstable solid electrolyte interface (SEI) formation occurs leading to lithium ion consumption

Engineering Contradiction:
Improvestructural stabilityVSAvoidSEI stability
Core Design Contradiction:
Stability of the object's compositionVSReliability

Solution Approach 1:

The patent applies pre-lithiated metal oxide as the outermost coating layer, which has been预先 treated with lithium. This preliminary lithium incorporation allows the SEI to form more stably during initial charging cycles, preventing the unstable SEI formation and subsequent lithium ion consumption that occurs with plain silicon oxide. The pre-lithiation compensates for initial lithium loss and promotes reliable SEI development.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The pre-lithiated metal oxide acts as an intermediary layer between the silicon oxide core and the electrolyte. This intermediate coating mediates the interaction between the electrode material and electrolyte, facilitating stable SEI formation while preventing direct contact that would cause unstable SEI and lithium ion consumption. The intermediary layer controls the interface chemistry to achieve reliable electrochemical performance.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Stability of the object's composition

If conventional coating technology is applied, then structural stability is improved, but capacity fading caused by volume expansion and unstable SEI formation is not fully resolved

Engineering Contradiction:
Improvestructural stabilityVSAvoidcapacity retention
Core Design Contradiction:
Stability of the object's compositionVSReliability

Solution Approach 1:

The patent changes the chemical composition parameter of the outermost coating layer by using pre-lithiated metal oxide instead of conventional non-lithiated coatings. This parameter change (incorporating lithium in the coating) directly addresses both volume expansion and SEI stability issues, leading to improved capacity retention. The compositional modification of the coating layer enables simultaneous resolution of multiple degradation mechanisms.

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent segments the protective function into multiple specialized layers: an inner conductive carbon layer for electrical conductivity and initial structural support, and an outer pre-lithiated metal oxide layer for SEI stabilization and volume expansion control. This segmentation of functions across layers allows each layer to optimize its specific role, achieving comprehensive protection against capacity fading that single-layer coatings cannot provide.

Inventive Principle:
Principle #1Segmentation

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 multi-layer composite structure enhances the stability and efficiency of lithium secondary batteries by preventing capacity fading and maintaining stable charging/discharging performance, reducing lithium ion trapping, and minimizing volume expansion.

Implementation Method 1

containing the pre-lithiated metal oxide formed through a lithiation reaction

Methodology Applied
Scientific EffectLithiation reaction: Chemical Bonding

Data Source

PatentUS12469844B2Multi-layer composite structure containing pre-lithiated metal oxide and method for preparing the same
Publication Date: 2025.11.11 KOREA UNIV RES & BUSINESS FOUND
  • US12469844B2 patent drawing
  • US12469844B2 patent drawing
  • US12469844B2 patent drawing

AI summary

A multi-layer composite structure containing a pre-lithiated metal oxide includes a negative electrode particle, a first coating layer disposed on the negative electrode particle and containing a conductive carbon material, and a second coating layer disposed on the first coating layer and containing the pre-lithiated metal oxide formed through a lithiation reaction.