Continuous Flow Graphene Gel Synthesis Without Pressurized Vessels

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Solution Overview

Problem

The hydrothermal gelation process for producing graphene monoliths requires high temperatures and pressures, making it difficult to scale up and leading to inhomogeneous microstructures and material instability due to the need for sealed pressurized vessels and batch processing.

Innovation Solution

A continuous flow synthesis method using a solvent with a boiling point higher than water, such as ethylene glycol, to deoxygenate graphene oxide and induce gelation, allowing for the formation of a graphene gel suspended in the solvent without the need for pressurized conditions, enabling continuous extrusion and subsequent drying to produce densified xerogels.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Temperature

If hydrothermal gelation is performed at high temperatures above water's boiling point, then graphene gel formation is achieved, but sealed pressurized vessels are required making batch processing difficult to scale up

Engineering Contradiction:
Improvereaction temperatureVSAvoidpressurized vessel requirement
Core Design Contradiction:
TemperatureVSDevice complexity

Solution Approach 1:

The patent changes the solvent parameter from water to a high-boiling-point solvent (ethylene glycol with boiling point 197°C). This parameter change allows the reaction to proceed at elevated temperatures without requiring pressurized vessels, as the solvent remains liquid at atmospheric pressure. The high boiling point of ethylene glycol enables thermal gelation of graphene oxide at temperatures that would normally require pressurization when using water.

Inventive Principle:
Principle #35Parameter changes

2Productivity

If larger reaction vessels are used to produce larger hydrogels, then production scale increases, but the hydrogels are prone to collapse due to their own weight

Engineering Contradiction:
Improveproduction scaleVSAvoidhydrogel structural stability
Core Design Contradiction:
ProductivityVSReliability

Solution Approach 1:

The patent performs preliminary crosslinking of graphene oxide sheets during the gelation process in ethylene glycol. This preliminary action creates a pre-reinforced gel network with enhanced mechanical strength before the hydrogel is removed from the solvent. The pre-established crosslinked structure provides sufficient structural support to prevent collapse when the hydrogel is transferred to air or water, enabling production of larger-scale hydrogels without structural failure.

Inventive Principle:
Principle #10Preliminary action

3Loss of time

If non-uniform drying is applied to hydrogels, then processing time is reduced, but cracking and inhomogeneous microstructures occur

Engineering Contradiction:
Improvedrying timeVSAvoidmicrostructure uniformity
Core Design Contradiction:
Loss of timeVSManufacturing precision

Solution Approach 1:

The patent performs preliminary crosslinking of the gel network during the gelation stage in ethylene glycol before the drying process. This pre-reinforced structure with enhanced mechanical strength can better withstand the stresses of rapid or non-uniform drying without developing cracks. The crosslinked network provides structural integrity that maintains microstructure uniformity even when drying conditions are not perfectly controlled, enabling faster processing without sacrificing 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

This method allows for the production of graphene gels and xerogels with controlled microstructures and improved mechanical properties, suitable for electrochemical applications like supercapacitors, without the limitations of high-pressure equipment, and can be scaled up for larger production.

Implementation Method 1

flowing a graphene oxide composition comprising graphene oxide and a solvent, the solvent having a boiling point higher than pure water, through a reaction chamber under conditions to deoxygenate the graphene oxide

Methodology Applied
Scientific EffectThermal deoxygenation: Thermolysis

Implementation Method 2

induce gelation to form a graphene gel suspended in the solvent

Methodology Applied
Scientific EffectGelation: Gel

Data Source

PatentUS11866337B2Methods for synthesizing graphene gels
Publication Date: 2024.01.09 NORTHWESTERN UNIV
  • US11866337B2 patent drawing
  • US11866337B2 patent drawing
  • US11866337B2 patent drawing

AI summary

Provided are methods for synthesizing a graphene gel. In embodiments, such a method comprises flowing a graphene oxide composition comprising graphene oxide and a solvent, the solvent having a boiling point higher than pure water, through a reaction chamber under conditions to deoxygenate the graphene oxide and induce gelation to form a graphene gel suspended in the solvent and flowing through the reaction chamber.