CVD Graphene Growth via Hydrogen Etching

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Solution Overview

Problem

Current methods for producing graphene by chemical vapor deposition (CVD) struggle to achieve controlled domain orientation and defined edge geometries, leading to structural defects in large-area films, which degrade the material's properties, and lack alignment with the underlying copper substrate.

Innovation Solution

A CVD process involving a high hydrogen-to-precursor flow ratio, where hydrogen etches graphene edges, allowing controlled growth of aligned domains on substrates with specific crystallographic orientations, such as copper, to produce high-quality single and bilayer graphene with defined edge geometries.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Shape

If atmospheric-pressure CVD is used to synthesize hexagonally shaped graphene domains, then defined zigzag edges can be achieved, but the domains are randomly oriented on the substrate resulting in structural defects

Engineering Contradiction:
Improveedge geometryVSAvoiddomain orientation control
Core Design Contradiction:
ShapeVSManufacturing precision

Solution Approach 1:

The patent applies parameter changes by utilizing low-pressure CVD conditions (1-100 mbar) instead of atmospheric pressure, which fundamentally alters the growth dynamics. This pressure parameter change enables controlled domain orientation and alignment with the copper substrate lattice, resolving the random orientation issue while preserving the hexagonal shape and zigzag edge geometry achieved in atmospheric CVD

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The patent implements local quality by creating different growth conditions for different regions of the substrate. By controlling the partial pressures of hydrogen and carbon precursor gases, the process achieves uniform domain orientation and alignment across the substrate surface, ensuring that each local region produces high-quality aligned domains rather than random orientations

Inventive Principle:
Principle #3Local quality

2Area of stationary object

If domains are allowed to grow and coalesce to form large-area films, then film coverage is improved, but structural defects are introduced that degrade material properties

Engineering Contradiction:
Improvefilm coverageVSAvoidmaterial properties
Core Design Contradiction:
Area of stationary objectVSReliability

Solution Approach 1:

The patent applies preliminary action by pre-aligning the graphene domains with the copper substrate lattice before coalescence occurs. The low-pressure CVD process promotes epitaxial growth where domains nucleate and orient themselves according to the underlying copper crystal structure. This preliminary alignment ensures that when domains coalesce to form large-area films, the grain boundaries are minimized and properly oriented, preventing structural defects that would otherwise degrade material properties

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent replaces the random thermal growth mechanism with a controlled epitaxial growth mechanism. By using low-pressure CVD with controlled gas flows and temperatures, the process substitutes uncontrolled domain formation with a mechanism where domain orientation is dictated by the crystallographic relationship between graphene and copper substrate, enabling defect-free large-area film formation

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

3Adaptability or versatility

If no correlation exists between graphene crystallographic orientation and copper grain orientation, then growth flexibility is maintained, but epitaxial relationship and alignment control are lost

Engineering Contradiction:
Improvegrowth flexibilityVSAvoidalignment control
Core Design Contradiction:
Adaptability or versatilityVSManufacturing precision

Solution Approach 1:

The patent applies parameter changes by operating at low pressures (1-100 mbar) which fundamentally alters the interaction between carbon precursor and copper substrate. This pressure parameter change enables the carbon atoms to diffuse and arrange themselves according to the copper lattice structure, establishing a strong epitaxial relationship. The controlled low-pressure environment maintains growth flexibility while simultaneously achieving precise alignment control through the copper-graphene crystallographic relationship

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

This process enables the production of high-quality graphene with controlled orientation and edge geometry, minimizing defects and enhancing mechanical and electronic properties, suitable for applications like transparent conducting electrodes and nanoelectronic devices.

Implementation Method 1

hydrogen etches graphene edges

Methodology Applied
Scientific EffectEtching:

Implementation Method 2

production of two-dimensional nanomaterials by chemical vapour deposition (CVD)

Methodology Applied
Scientific EffectChemical vapour deposition: Chemical Vapour Deposition

Implementation Method 3

the precursor reacts in the chamber to form said material on a surface of the substrate

Methodology Applied
Scientific EffectDecomposition: Decomposition (biological)

Implementation Method 4

epitaxial relationship exists between the substrate and graphene layer

Methodology Applied
Scientific EffectEpitaxy: Epitaxy

Data Source

PatentUS9399581B2Process for producing two-dimensional nanomaterials
Publication Date: 2016.07.26 OXFORD UNIVERSITY INNOVATION LTD
  • US9399581B2 patent drawing
  • US9399581B2 patent drawing
  • US9399581B2 patent drawing

AI summary

The present invention provides a process for producing a two-dimensional nanomaterial by chemical vapor deposition (CVD), the process comprising contacting a substrate in a reaction chamber with a first flow which contains hydrogen and a second flow which contains a precursor for said material, wherein the contacting takes place under conditions such that the precursor reacts in the chamber to form said material on a surface of the substrate, wherein the ratio of the flow rate of the first flow to the flow rate of the second flow is at least 5:1. Two-dimensional nanomaterials obtainable by said process are also provided, as well as devices comprising said nanomaterials.