A robust and reproducible procedure for cross-linking thermoset polymers using molecular simulation

Area of Science:

• Materials Science
• Computational Chemistry
• Polymer Science

Background:

• Molecular simulation is crucial for linking polymer structure to function, enabling material design.
• Simulating thermoset polymers, like epoxies, faces challenges in preparing polymerized samples.
• A robust, reproducible method for generating cross-linked epoxy structures for simulation is needed.

Purpose of the Study:

• To introduce a clear, reproducible cross-linking protocol for generating 3D epoxy polymer structures.
• To enable reliable molecular simulations of thermoset polymers, applicable to general cases.
• To establish a benchmark protocol for simulating epoxy polymers and related systems.

Main Methods:

• Developed a reproducible procedure for calculating partial atomic charges.
• Implemented a reliable process for generating and validating equilibrated liquid precursor mixtures.
• Established a novel, robust protocol for generating 3D cross-linked solid polymer structures.

Main Results:

• Successfully generated reproducible 3D cross-linked epoxy polymer structures.
• Utilized generated structures for molecular dynamics simulations to calculate thermo-mechanical properties.
• Simulated properties showed favorable comparison with experimental data.

Conclusions:

• The developed protocol provides a benchmark for simulating epoxy polymers.
• The method is detailed, reproducible, and applicable to general thermoset polymers.
• The protocol can be adapted for modeling dynamically cross-linked epoxy samples with surfaces and nanostructures.