Graphene Growth on Oriented Copper Foil via Pulse Electroplating

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Solution Overview

Problem

Existing methods for producing graphene using copper foils face challenges in achieving uniform monolayer growth due to non-uniform surface energy and low reactivity, leading to the formation of multilayer graphene islands, which hinders industrial-scale application.

Innovation Solution

A method involving the formation of unidirectionally oriented step structures on a face-centered cubic metal catalyst substrate, specifically copper, silver, or gold, using pulse wave current electroplating and annealing in a hydrogen atmosphere to create a uniform surface energy state conducive to monolayer graphene growth.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If general copper foils are used as catalyst substrate, then the manufacturing process is simple and easy to implement, but the surface energy is non-uniform leading to multilayer graphene formation instead of uniform monolayer growth

Engineering Contradiction:
Improveease of manufactureVSAvoiduniformity of graphene layer
Core Design Contradiction:
Ease of manufactureVSManufacturing precision

Solution Approach 1:

The copper foil substrate undergoes preliminary treatment including electropositive treatment and formation of step structures before the actual graphene growth process. This preliminary preparation creates a uniform surface energy distribution and appropriate nucleation sites, enabling subsequent uniform monolayer graphene growth while maintaining the simplicity of using copper foil as substrate.

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

Step structures are formed on the copper foil surface to create local variations in surface energy and atomic arrangement. These localized step structures serve as preferential nucleation sites for graphene growth, ensuring uniform monolayer formation across the entire substrate while maintaining the overall simplicity of the copper foil-based approach.

Inventive Principle:
Principle #3Local quality

2Manufacturing precision

If single crystalline metals with specific orientations are used to achieve uniform energy state, then uniform graphene growth is improved, but the device complexity and manufacturing difficulty increase significantly

Engineering Contradiction:
Improveuniformity of graphene layerVSAvoidcomplexity of catalyst preparation
Core Design Contradiction:
Manufacturing precisionVSDevice complexity

Solution Approach 1:

The invention uses commercially available polycrystalline copper foil as the catalyst substrate instead of requiring expensive and complex single crystalline metals. The copper foil is disposed of after use, and its simplicity and low cost enable uniform graphene growth without the need for complex catalyst preparation processes.

Inventive Principle:
Principle #27Cheap short-living objects (Disposable)

Solution Approach 2:

The invention changes the surface properties of the copper foil through electropositive treatment and step structure formation, rather than requiring changes in the bulk crystal structure. This parameter change at the surface level achieves uniform energy state and controlled nucleation while maintaining the simplicity and low cost of using polycrystalline copper foil.

Inventive Principle:
Principle #35Parameter changes

3Stability of the object's composition

If copper catalyst is used with low carbon solubility, then the catalyst stability is maintained, but the adsorption rate of carbon atoms becomes difficult to control leading to non-uniform growth

Engineering Contradiction:
Improvestability of catalystVSAvoidcontrol of carbon adsorption
Core Design Contradiction:
Stability of the object's compositionVSManufacturing precision

Solution Approach 1:

The copper catalyst undergoes preliminary electropositive treatment and step structure formation to create uniform surface energy distribution and controlled nucleation sites. This preliminary action enables precise control of carbon atom adsorption at the surface while maintaining the low bulk solubility and stability of the copper catalyst throughout the growth process.

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

This approach enables the uniform and epitaxial growth of graphene, increasing the growth rate and ensuring 95% or more of the graphene produced is in the form of monolayer films, making it suitable for industrial applications.

Implementation Method 1

the atomic packing density of a metal varies depending on the orientation of the metal and because factors, including dislocation density, stacking fault energy, twins and impurities, which influence the surface energy of the catalyst, influence the reaction with the gaseous molecules or atoms to be adsorbed

Methodology Applied
Scientific EffectAdsorption: Adsorption

Implementation Method 2

forming step structures on the alloyed metal catalyst substrate in the atmosphere of hydrogen gas and a gas having a molecular weight higher than the atomic weight of carbon

Methodology Applied
Scientific EffectAnnealing: Annealing

Data Source

PatentUS10253409B2Method of manufacturing graphene using metal catalyst
Publication Date: 2019.04.09 SRC CO LTD
  • US10253409B2 patent drawing
  • US10253409B2 patent drawing
  • US10253409B2 patent drawing

AI summary

The present invention relates to a method for producing graphene on a face-centered cubic metal catalyst having a plane oriented in one direction, and more particularly to a method of producing graphene on a metal catalyst having the (100) or (111) crystal structure and a method of producing graphene using a catalyst metal foil having a single orientation, obtained by electroplating a metal catalyst by a pulse wave current and annealing the metal catalyst. The invention also relates to a method of producing graphene using a metal catalyst, and more particularly to a method of producing graphene, comprising the steps of: alloying a metal catalyst with an alloying element; forming step structures on the metal catalyst substrate in an atmosphere of a gas having a molecular weight of carbon; and supplying hydrocarbon and hydrogen gases to the substrate. On unidirectionally oriented metal catalyst prepared according to the present invention, graphene can be grown uniformly and epitaxially. Moreover, a method for producing graphene according to the present invention can form monolayer graphene by epitaxially growing graphene while increasing the growth rate of graphene.