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Understanding Interlayer Adhesion in Lamellar Polymer Composite Materials via Computation.

Ahmed H Ibrahim¹, Mark DelloStritto^1,2, Subhajit Acharya²

¹Temple Materials Institute, Temple University, Philadelphia, Pennsylvania 19122, United States.

ACS Polymers Au

|February 16, 2026

Summary

Improving body armor involves enhancing polymer composites like poly(p-phenylene terephthalamide) (PPTA) and ultrahigh-molecular-weight polyethylene (UHMWPE). Coating with polypyrrole (PPy) significantly boosts PPTA/UHMWPE adhesion more than plasma treatment, crucial for better ballistic performance.

Keywords:

adhesion composites molecular dynamics polymers strength

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Area of Science:

Materials Science
Polymer Science
Computational Materials Science

Background:

High-performance polymers like poly(p-phenylene terephthalamide) (PPTA) and ultrahigh-molecular-weight polyethylene (UHMWPE) are key in body armor.
Composite materials offer enhanced properties by combining different polymers, allowing tunable thickness, weight, and rigidity.
Optimizing interfaces in polymer composites is critical for improving overall material performance, especially in ballistic applications.

Purpose of the Study:

To investigate strategies for modifying the PPTA/UHMWPE interface to enhance adhesion and ballistic performance.
To compare the effectiveness of plasma treatment versus polypyrrole (PPy) coating on PPTA/UHMWPE adhesion.
To understand the molecular mechanisms governing interfacial adhesion between PPTA and UHMWPE.

Main Methods:

Fully atomistic molecular dynamics (MD) simulations were employed to model polymer interfaces.
Peel test experiments and imaging were conducted to experimentally validate simulation findings.
Density functional theory (DFT) calculations were used to analyze electronic structure and binding energies.

Main Results:

Plasma treatment of UHMWPE enhanced adhesion to PPTA, but PPy coating proved more effective.
DFT calculations revealed that polar interactions of pyrrole moieties and hydrogen bonds contribute significantly to binding energy.
Experimental results showed that PPy nanostructures performed better as nanofibers than nanodomains, indicating the importance of surface area and interaction site density.

Conclusions:

Interfacial adhesion depends on both specific polymer monomer interactions and the accessible surface area.
Achieving optimal adhesion requires balancing interaction strength with the density of interaction sites.
Polypyrrole coating, particularly in nanofiber form, presents a promising strategy for enhancing PPTA/UHMWPE composites for improved ballistic performance.