Pristine Graphene from Kish Graphite via Acid Intercalation

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Solution Overview

Problem

Current methods for producing graphene from Kish graphite result in materials with significant defects and low yield, failing to achieve pristine graphene with high purity and minimal oxygen, nitrogen, and hydrogen content.

Innovation Solution

A method involving the intercalation of Kish graphite with a nitrate salt and acid, followed by thermal expansion and ultra-sonication, to produce pristine graphene with less than 5% oxygen, nitrogen, and 0.5% hydrogen, using a process that includes sieving, flotation, acid leaching, and centrifugation for separation.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If mechanical liquid exfoliation is used to produce graphene, then the process is simple, but the yield is very low (5-10%) and the graphene quality is poor with defects

Engineering Contradiction:
Improveprocess simplicityVSAvoidgraphene yield
Core Design Contradiction:
Ease of manufactureVSProductivity

Solution Approach 1:

The invention changes the chemical parameters by using specific acid mixtures (sulfuric acid, nitric acid, phosphoric acid) and controlling oxidation time and temperature to transform graphite into high-quality graphene oxide with improved exfoliation properties, thereby increasing yield and reducing defects

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The invention utilizes phase transition by converting graphite to graphite oxide through chemical oxidation, then exfoliating it to graphene oxide, and finally reducing it back to graphene. This multi-phase transformation process improves both yield and quality compared to direct mechanical exfoliation

Inventive Principle:
Principle #36Phase transitions

2Manufacturing precision

If chemical oxidation methods (Hummer method) are used to produce graphene oxide, then the exfoliation is improved, but the graphene contains significant oxygen groups and defects

Engineering Contradiction:
Improveexfoliation qualityVSAvoidgraphene purity
Core Design Contradiction:
Manufacturing precisionVSReliability

Solution Approach 1:

The invention optimizes oxidation parameters by using a specific mixture of acids (sulfuric, nitric, phosphoric) in controlled ratios and conditions, then implements a reduction step to remove excess oxygen groups, achieving a balance between exfoliation quality and graphene purity with less than 5% oxygen content

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The invention extracts and removes harmful oxygen groups and impurities through the reduction step after oxidation, separating the desired graphene structure from the unwanted oxygen-containing functional groups to improve overall purity

Inventive Principle:
Principle #2Taking out (Extraction)

3Productivity

If CVD method is used to produce graphene, then the graphene can be obtained, but it includes many defects such as foreign atoms sitting in place of carbon

Engineering Contradiction:
Improvegraphene productionVSAvoidgraphene quality
Core Design Contradiction:
ProductivityVSManufacturing precision

Solution Approach 1:

The invention uses self-service by starting with high-purity kish graphite as the carbon source, which already contains the correct carbon structure. The chemical oxidation and reduction process maintains the carbon lattice integrity without introducing foreign atoms, allowing the material to essentially build itself into high-quality graphene

Inventive Principle:
Principle #25Self-service

4Device complexity

If microwave expansion is used for graphite intercalation compound, then the expansion can be achieved, but it is difficult to control the expansion degree and the process is time-consuming (overnight intercalation)

Engineering Contradiction:
Improveexpansion capabilityVSAvoidprocess time
Core Design Contradiction:
Device complexityVSLoss of time

Solution Approach 1:

The invention changes the expansion mechanism from microwave heating to controlled thermal expansion using conventional heating methods. By adjusting temperature and time parameters during the oxidation and drying steps, the expansion degree is precisely controlled without requiring overnight intercalation, significantly reducing process time while maintaining effectiveness

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 method significantly improves the purity and yield of pristine graphene, achieving high-quality single-layer carbon atoms in a honeycomb lattice with minimal impurities, suitable for industrial applications in metal industries.

Implementation Method 1

the intercalation of kish graphite with a nitrate salt and an acid to obtain intercalated kish graphite

Methodology Applied
Scientific EffectIntercalation: Diffusion

Implementation Method 2

the thermal expansion of the intercalated kish graphite to obtain expanded kish graphite at a temperature above 600° C.

Methodology Applied
Scientific EffectThermal expansion: Thermal Expansion

Implementation Method 3

the exfoliation by ultra-sonication to obtain exfoliated kish graphite

Methodology Applied
Scientific EffectUltrasonic vibration: Ultrasonic Vibration

Implementation Method 4

the separation of the unexfoliated kish graphite and the obtained pristine graphene

Methodology Applied
Scientific EffectCentrifugal separation: Centrifugal Separation

Data Source

PatentUS11535519B2Method for the manufacture of pristine graphene from Kish graphite
Publication Date: 2022.12.27 ARCELORMITTAL SA
  • US11535519B2 patent drawing

AI summary

A method for the manufacture of pristine graphite from Kish graphite including three different steps A, B and C; the pristine obtained with among others a high amount of carbon atoms, i.e. a pristine graphene having a high purity; and the use of this pristine graphene.