Falling-Leaves Stacking Aggregation of Two-Dimensional Macromolecular Graphene Oxide in Solution

Area of Science:

• Materials Science
• Physical Chemistry
• Chemical Engineering

Background:

• Understanding 2D macromolecule dynamics is key for material performance.
• Limited knowledge exists on how macromolecular sheets assemble in solution.
• Lack of quantitative assembly description hinders structural control.

Purpose of the Study:

• Investigate aggregation thermodynamics and kinetics of 2D macromolecules.
• Model the assembly process using single-layer graphene oxide (GO) as a case study.
• Develop a quantitative description for controlling assembled material structures.

Main Methods:

• Applied Flory-Huggins theory combined with experimental observations.
• Utilized single-layer graphene oxide (GO) as a model system.
• Developed a theoretical falling-leaf model for kinetic aggregation.

Main Results:

• Unveiled a critical thermodynamic transition of GO dependent on solvent properties.
• Proposed a quantitative falling-leaf model for 2D sheet aggregation kinetics.
• Validated that GO aggregate thickness follows a power law with poor solvent content.

Conclusions:

• Provided fundamental insights into the phase separation of 2D macromolecules.
• Offered a method to modulate the aggregated structures of assembled materials.
• Established a quantitative framework for understanding and controlling macromolecular assembly.