Flexible Graphene Paper via Electrochemical Exfoliation

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Solution Overview

Problem

There is a need for an efficient, cost-effective, and environmentally low-impact method to produce free-standing, flexible, and highly conductive electrochemically exfoliated graphene paper.

Innovation Solution

The method involves passing an electric potential between a graphite-containing anode and cathode in a buffered aqueous electrolyte to exfoliate partially oxidized graphene, which is then separated, acidified, and dried to yield free-standing graphene sheets with a high carbon-to-oxygen ratio, suitable for scalable production.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Object-affected harmful factors

If conventional electrochemical exfoliation methods are used to produce graphene flakes, then environmental friendliness is improved, but manufacturing efficiency and scalability are insufficient

Engineering Contradiction:
Improveenvironmental impactVSAvoidmanufacturing efficiency
Core Design Contradiction:
Object-affected harmful factorsVSProductivity

Solution Approach 1:

The patent extracts and removes oxygen-containing functional groups from graphene oxide through controlled electrochemical reduction. This selective extraction of harmful oxygen groups improves the electrical conductivity and reduces environmental impact while maintaining the eco-friendly nature of the process, resolving the contradiction between environmental friendliness and manufacturing efficiency

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The patent employs controlled electrochemical reduction by adjusting electrical parameters (voltage, current, time) to precisely control the reduction degree of graphene oxide. This parameter control enables scalable production while maintaining environmental friendliness, as the process can be optimized for both efficiency and low environmental impact

Inventive Principle:
Principle #35Parameter changes

2Reliability

If graphene oxide is reduced using chemical reducing agents, then conductivity is improved, but environmental harm increases due to toxic agents

Engineering Contradiction:
Improveelectrical conductivityVSAvoidenvironmental harm
Core Design Contradiction:
ReliabilityVSObject-affected harmful factors

Solution Approach 1:

The patent replaces chemical reducing agents with electrochemical reduction using electricity as the reducing power. This substitution eliminates toxic chemicals while maintaining effective reduction of graphene oxide, achieving high conductivity without environmental harm from toxic agents

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

Solution Approach 2:

The electrochemical reduction process uses electrons directly from the electrode to reduce graphene oxide, eliminating the need for external chemical reducing agents. This self-service approach achieves high conductivity improvement while avoiding environmental contamination from toxic chemicals

Inventive Principle:
Principle #25Self-service

3Strength

If vacuum filtration is used to fabricate graphene paper, then structural integrity is improved, but production cost and complexity increase

Engineering Contradiction:
Improvestructural integrityVSAvoidproduction complexity
Core Design Contradiction:
StrengthVSDevice complexity

Solution Approach 1:

The patent segments the fabrication process into distinct stages: electrochemical exfoliation, filtration, drying, and optional reduction. This segmentation allows each step to be optimized independently, maintaining structural integrity through controlled filtration while reducing overall process complexity and enabling easier scaling

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The patent performs preliminary electrochemical exfoliation to create well-dispersed graphene oxide flakes before filtration. This preliminary action ensures uniform distribution and proper morphology, which maintains structural integrity during subsequent filtration while simplifying the overall process by preventing aggregation issues

Inventive Principle:
Principle #10Preliminary action

4Productivity

If high oxidation levels are used during electrochemical exfoliation, then exfoliation efficiency is improved, but carbon-to-oxygen ratio decreases affecting conductivity

Engineering Contradiction:
Improveexfoliation efficiencyVSAvoidelectrical conductivity
Core Design Contradiction:
ProductivityVSReliability

Solution Approach 1:

The patent employs periodic electrochemical reduction after oxidation to restore conductivity. This periodic action alternates between oxidation (for exfoliation efficiency) and reduction (for conductivity recovery), achieving both high exfoliation efficiency and maintained electrical conductivity through cyclic treatment

Inventive Principle:
Principle #19Periodic action

Solution Approach 2:

The patent controls the oxidation level by adjusting electrochemical parameters (voltage, time, current density) to achieve optimal exfoliation while maintaining adequate carbon-to-oxygen ratio. This parameter optimization ensures both high exfoliation efficiency and sufficient electrical conductivity without excessive oxidation

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 method produces high-performance, flexible graphene paper with superior mechanical and electrochemical qualities, including high electrical conductivity and specific capacitance, suitable for applications in supercapacitors, lithium-ion batteries, and solar cells, while being environmentally friendly and cost-effective.

Implementation Method 1

partially oxidized graphene is exfoliated from the anode and/or the cathode into the electrolyte

Methodology Applied
Scientific EffectOxidation: Oxidation

Implementation Method 2

partially oxidized graphene is exfoliated from the anode and/or the cathode into the electrolyte

Methodology Applied
Scientific EffectReduction: Reduction

Implementation Method 3

passing an electric potential between a graphite-containing anode and a graphite-containing cathode disposed in a buffered aqueous electrolyte

Methodology Applied
Scientific EffectElectrolysis: Electrolysis

Data Source

PatentUS11091844B2Method to make flexible, free-standing graphene paper and product formed thereby
Publication Date: 2021.08.17 WISCONSIN ALUMNI RES FOUND
  • US11091844B2 patent drawing
  • US11091844B2 patent drawing
  • US11091844B2 patent drawing

AI summary

A method to make free-standing graphene sheets and the free-standing graphene sheets so formed. The method includes the steps of exfoliating partially oxidized graphene from a carbon-containing electrode into an aqueous solution, acidifying the aqueous solution, and separating from the acidified solution partially oxidized graphene sheet. The partially oxidized graphene is then dried to yield free-standing graphene sheet having a carbon-to-oxygen ratio of at least about 8.0.