Elucidating the impact of microstructure on mechanical properties of phase-segregated polyurea: Finite element modeling of molecular dynamics derived microstructures

TL;DR

This study develops a finite element model to predict how microstructural differences in phase-segregated polyurea influence its mechanical properties, aligning simulations with experimental SAXS data.

Contribution

The paper introduces a novel finite element modeling framework that incorporates phase-specific constitutive laws and microstructure evolution to predict polyurea behavior.

Findings

Model accurately predicts mechanical response under various loading conditions.

Microstructure transformations in polyurea mirror SAXS experimental results.

Differences in elastomeric phase length explain variations in mechanical properties.

Abstract

Phase-segregated polyureas (PU) have received considerable interest due to their use as tough, impact-resistant coatings. Polyureas are favored for these applications due to their mechanical strain rate sensitivity and energy dissipation. Predicting and tailoring the mechanical response of PU remains challenging due to the complex interaction between its elastomeric and glassy phases. To elucidate the role of PU microstructure on its mechanical properties, we developed a finite element modeling framework in which each phase is represented by a volume fraction within a representative volume element (RVE). Critically, we used separate constitutive models to describe the elastomeric and glassy phases. We developed a plasticity-driven breakdown process in which we model the glassy phase disaggregating into a new phase. The overall contribution of each phase at a material point is determined by their respective volume fractions within the RVE. We applied our modeling methods to two compositions of PU with differing elastomeric segment lengths derived from oligoether diamines, Versalink P650 and P1000. Our simulations show that a combination of microstructural differences and elastomeric phase properties accounts for the difference in mechanical response between P650 and P1000. We show our model's ability to predict PU behavior in various loading conditions, including low-rate cyclic loading and monotonic loading over a wide range of strain rates. Our model produces microstructure transformations that mirror those indicated by small-angle X-ray scattering (SAXS) experiments. Fourier transform analysis of our RVEs reveals glassy phase fibrillation due to deformation, a finding consistent with SAXS experiments.