Silicon Oxide Composite Anode for Swelling-Stable Lithium Batteries

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Solution Overview

Problem

Lithium secondary batteries face challenges with silicon-based negative electrodes due to rapid volumetric swelling and shrinking, leading to electrode cracking, low initial charge efficiency, and reduced cycle life, which affects battery capacity and weight efficiency.

Innovation Solution

A silicon-silicon oxide-magnesium silicate composite is developed, comprising a silicon oxide matrix with Si, MgSiO3, and Mg2SiO4 crystal grains, where the content ratio and crystal sizes of these components are optimized to enhance initial efficiency and cycle characteristics, and a method involving a vapor-phase reaction and heat treatment is used to produce the composite.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon-based negative electrode is used to achieve high theoretical capacity (4200 mAh/g), then battery capacity is improved, but volumetric swelling to 300% or more causes cracking and separation leading to rapid degradation of cycle life

Engineering Contradiction:
Improvebattery capacityVSAvoidcycle life
Core Design Contradiction:
Quantity of substanceVSReliability

Solution Approach 1:

Silicon particles are embedded within a silicon oxide matrix, creating a nested structure where the inner silicon provides high capacity while the outer silicon oxide shell constrains volumetric expansion and prevents particle cracking, resolving the contradiction between high capacity and cycle life

Inventive Principle:
Principle #7Nested doll (Nesting)

Solution Approach 2:

A composite material consisting of silicon and silicon oxide in specific ratios (0.1-10 wt% silicon, 99.9-90 wt% silicon oxide) is created, combining the high capacity advantage of silicon with the structural stability of silicon oxide to simultaneously achieve high capacity and long cycle life

Inventive Principle:
Principle #40Composite materials

2Reliability

If silicon oxide-based negative electrode is used to reduce volumetric swelling ratio, then cycle life characteristics are improved, but capacity is reduced to approximately half of silicon-based electrode

Engineering Contradiction:
Improvecycle life characteristicsVSAvoidbattery capacity
Core Design Contradiction:
ReliabilityVSQuantity of substance

Solution Approach 1:

The electrode structure is designed with local quality variation: silicon-rich regions (0.1-10 wt%) provide high capacity in specific locations, while silicon oxide-dominated regions (99.9-90 wt%) provide structural stability, creating a heterogeneous structure that optimizes both capacity and cycle life locally

Inventive Principle:
Principle #3Local quality

3Use of energy by moving object

If silicon oxide reacts with lithium during initial charge to produce lithium oxide and lithium silicate, then electrochemical reaction occurs, but lithium oxide cannot participate in subsequent reactions causing irreversible reaction and depletion of lithium

Engineering Contradiction:
Improveelectrochemical reactionVSAvoidlithium depletion
Core Design Contradiction:
Use of energy by moving objectVSLoss of substance

Solution Approach 1:

The composition parameters of the negative electrode are precisely controlled, with silicon content limited to 0.1-10 wt% and silicon oxide content at 99.9-90 wt%, optimizing the balance between initial electrochemical activation and minimizing irreversible lithium consumption throughout cycling

Inventive Principle:
Principle #35Parameter changes

4Quantity of substance

If silicon-based negative electrode is used to achieve high capacity, then battery capacity is improved, but weight efficiency is reduced due to excessive capacity requirements of positive electrode

Engineering Contradiction:
Improvebattery capacityVSAvoidweight efficiency
Core Design Contradiction:
Quantity of substanceVSWeight of moving object

Solution Approach 1:

The negative electrode composition is optimized with silicon content at 0.1-10 wt% and silicon oxide at 99.9-90 wt%, achieving high capacity with reduced irreversible lithium consumption, which allows the positive electrode capacity to be better matched and improves overall battery weight efficiency

Inventive Principle:
Principle #35Parameter changes

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 achieves high battery capacity, excellent cycle characteristics, and improved charge/discharge efficiency, minimizing electrode degradation and maintaining performance over multiple cycles.

Implementation Method 1

a method involving a vapor-phase reaction and heat treatment is used to produce the composite

Methodology Applied
Scientific EffectVapor-phase reaction: Chemical Vapour Deposition

Data Source

PatentUS11942640B2Negative electrode active material for lithium secondary battery and lithium secondary battery comprising the same
Publication Date: 2024.03.26 LG ENERGY SOLUTION LTD

AI summary

Provided is a negative electrode active material for a lithium secondary battery which includes: a silicon-silicon oxide-magnesium silicate composite comprising a silicon oxide (SiOx, 0<x≤2) matrix; and silicon (Si) crystal grains, MgSiO3 crystal grains and Mg2SiO4 crystal grains present in the silicon oxide matrix, wherein the MgSiO3 crystal grains have a crystal size of 5-30 nm and the Mg2SiO4 crystal grains have a crystal size of 20-100 nm in the silicon-silicon oxide-magnesium silicate composite, and the content ratio of MgSiO3 crystal grains to Mg2SiO4 crystal grains is 2:1-1:1 on the weight basis. A method for preparing the negative electrode active material for a lithium secondary battery is also provided.