Polyolefin blends with co-continuous architectures enabled by dynamic covalent crosslinking

作者：Eliza K. Neidhart, Stephanie M. Ribet, Taehyun A. Lee, Logan T. Kearney, Karen C. Bustillo, Eric A. Dailing, Mutian Hua, Colin Ophus, Sophia N. Fricke, Ah-Young Song, Jeffrey A. Reimer, Erik J. Alexanian, Joanna M. Atkin, Brett A. Helms, Frank A. Leibfarth · 发表于：Science Advances · 年份：2026 · DOI：10.1126/sciadv.aee2328 · 被引用次数：1 · 研究领域：Advanced Polymer Synthesis and Characterization、Polymer composites and self-healing、Polymer crystallization and properties

Blending polymers produces brittle materials due to macrophase separation and poor interfacial adhesion, which is exemplified by mixtures of polyolefins. This presents a formidable challenge for the mechanical recycling of mixed plastic waste. Here, we demonstrate that dynamic covalent crosslinking of immiscible polyolefin blends creates macrophase separated co-continuous architectures, yet they display excellent mechanical properties, which challenges the conventional wisdom regarding morphology-property relationships in polymer blend compatibilization. We find that the position and orientation of dynamic crosslinks and their influence on crystallinity are key to understanding the structure-morphology-property relationships. In particular, high-resolution microscopy imaging reveals alignment of crystallite planes with strong orientational preference, particularly at polymer-polymer interfaces, which contribute to material performance. We further demonstrate that changes in crosslinker density and valency allow the properties of binary and ternary polyolefin blends to be tuned in a modular fashion.