Reduced Graphene Oxide-Silicon Core-Shell Anode for Volume Expansion

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Solution Overview

Problem

The commercialization of silicon as a high-capacity anode active material for lithium secondary batteries is hindered by its large volume expansion and structural breakdown during lithium ion absorption, leading to reduced initial efficiency and cycle characteristics.

Innovation Solution

A reduced-graphene-oxide/silicon-metal-particle composite with a core-shell structure is manufactured using a graphene oxide dispersion solution formed through cation-pi interaction, where reduced graphene oxide is added to a polymer with silicon metal particles and dried, eliminating the need for a reduction process and enhancing dispersibility, thereby forming a stable composite powder for use in secondary battery electrodes.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Quantity of substance

If silicon metal particles are used as anode active material, then capacity per unit weight and volume is improved, but volume expansion and structural breakdown occur during lithium ion absorption

Engineering Contradiction:
Improvecapacity per unit weight and volumeVSAvoidstructural stability during lithium ion absorption
Core Design Contradiction:
Quantity of substanceVSStability of the object's composition

Solution Approach 1:

A flexible polymer shell is formed around silicon metal particles through coating in a polymer solution containing dispersed reduced graphene oxide. This shell accommodates volume expansion during lithium ion absorption while maintaining structural integrity, preventing particle breakdown and preserving capacity over multiple charge-discharge cycles.

Inventive Principle:
Principle #30Flexible shells and thin films

Solution Approach 2:

A composite structure is created by combining silicon metal particles with a polymer matrix containing reduced graphene oxide. The polymer provides mechanical flexibility to handle volume changes, while the reduced graphene oxide enhances electrical conductivity and structural stability, creating a synergistic composite that maintains both high capacity and structural integrity.

Inventive Principle:
Principle #40Composite materials

2Reliability

If graphene oxide is reduced through heat treatment, then reduced graphene oxide is formed, but metal particles may be oxidized

Engineering Contradiction:
Improvereduced graphene oxide formationVSAvoidmetal particle oxidation
Core Design Contradiction:
ReliabilityVSObject-affected harmful factors

Solution Approach 1:

The thermal reduction process is replaced with a chemical reduction method using sodium borohydride in an aqueous solution. This chemical reduction occurs at room temperature or low temperatures, avoiding the high heat treatment that would cause metal particle oxidation, while still successfully forming reduced graphene oxide with the desired properties.

Inventive Principle:
Principle #28Mechanics substitution (Replace mechanical system)

Solution Approach 2:

The reduction conditions are changed from high-temperature thermal processing to low-temperature chemical reduction. By changing the temperature parameter and the chemical mechanism, the process achieves reduced graphene oxide formation without exposing metal particles to oxidizing conditions that would occur during heat treatment.

Inventive Principle:
Principle #35Parameter changes

3Reliability

If conventional manufacturing process is used, then graphene-wrapped metal particles are formed, but manufacturing process becomes complicated

Engineering Contradiction:
Improvegraphene-wrapped metal particles formationVSAvoidmanufacturing process complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

Multiple process steps are merged into a single coating operation. The polymer solution containing pre-dispersed reduced graphene oxide is applied directly to the silicon metal particles in one step, combining the dispersion, coating, and reduced graphene oxide formation processes into a single manufacturing operation, thereby simplifying the overall process.

Inventive Principle:
Principle #5Merging (Combining)

Solution Approach 2:

Reduced graphene oxide is pre-dispersed in the polymer solution before the coating process. This preliminary preparation ensures uniform distribution and eliminates the need for subsequent reduction steps or complex multi-stage processing, simplifying the manufacturing workflow while ensuring consistent product quality.

Inventive Principle:
Principle #10Preliminary action

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 powder maintains high capacity and stability by preventing silicon volume expansion and structural breakdown, improving the reversibility and cycle characteristics of lithium secondary batteries.

Implementation Method 1

graphene oxide formed through cation-pi interaction

Methodology Applied
Scientific EffectCation-pi interaction:

Implementation Method 2

added to a polymer for dispersion along with silicon metal particles, and then dried

Methodology Applied
Scientific EffectEvaporation: Evaporation

Data Source

PatentUS11742473B2Reduced graphene oxide-silicon metal particle complex, complex manufacturing method, and secondary battery electrode comprising complex
Publication Date: 2023.08.29 KOREA ELECTROTECH RES INST
  • US11742473B2 patent drawing
  • US11742473B2 patent drawing
  • US11742473B2 patent drawing

AI summary

The present invention relates to a reduced-graphene-oxide/silicon-metal-particle composite, a method of manufacturing the composite and an electrode for a secondary battery including the composite. The method of manufacturing the reduced-graphene-oxide/silicon-metal-particle composite includes preparing a reduced-graphene-oxide dispersion solution by reducing graphene oxide formed through cation-pi interaction, preparing a reduced-graphene-oxide/silicon-metal-particle dispersion solution by mixing the reduced-graphene-oxide dispersion solution with silicon metal particles, and manufacturing a composite powder having a core-shell structure by drying the reduced-graphene-oxide/silicon-metal-particle dispersion solution. Thereby, reduced graphene oxide can be formed using the graphene oxide dispersion solution having few defects and high purity obtained through cation-pi interaction, and dried to afford a composite powder having a core-shell structure, which is applicable to an electrode for a secondary battery.