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Probing Viscoelastic Properties and Interfaces in High-Density Polyethylene Vitrimers at the Nanoscale Using Dynamic
Lanti Yang1, Pierre Nickmilder2, Henk Verhoogt3
1Analytical Science Europe, Corporate T&I, SABIC, Plasticslaan 1, Bergen op Zoom 4612 PX, The Netherlands.
ACS Applied Materials & Interfaces
|July 12, 2024
Summary
This study reveals distinct nanostructures in high-density polyethylene (HDPE) vitrimers using advanced atomic force microscopy (AFM). These findings explain improved bulk properties, offering insights into vitrimer material science.
Area of Science:
- Polymer Science and Engineering
- Materials Science and Nanotechnology
Background:
- Vitrimers offer a unique combination of thermoset and thermoplastic properties.
- Understanding the nanoscale structure and interfaces in vitrimers is crucial but challenging.
- Dynamic cross-linking significantly influences vitrimer viscoelastic behavior.
Purpose of the Study:
- To characterize the nanoscale viscoelastic properties and interfaces in high-density polyethylene (HDPE) vitrimers.
- To investigate the correlation between vitrimer nanostructure and bulk material behavior.
Main Methods:
- Utilized dynamic modes of atomic force microscopy (AFM), including intermodulation AFM (ImAFM) and AFM-based dynamic mechanical analysis (AFM-nDMA).
- Employed k-means clustering algorithm for phase analysis.
- Quantified local viscoelastic properties and adhesion forces at the nanoscale.
Main Results:
- Identified two distinct phases with differing viscoelastic properties in the HDPE vitrimer system.
- Revealed a cross-linking-rich network structure within a cross-linking-poor matrix at the nanoscale.
- Observed higher adhesion forces in the cross-linking-rich regions compared to the matrix.
Conclusions:
- The nanoscale heterogeneity and viscoelastic properties of HDPE vitrimers are elucidated.
- Findings provide explanations for enhanced bulk properties such as decreased crystallinity and increased dimensional stability.
- This research offers critical insights into the structure-property relationships governing vitrimer behavior.

