Thermally Reversible and Recyclable Polyethylene Networks via Furan–Maleimide Diels–Alder Dynamic Covalent Chemistry

Authors

• Zengheng Hao, China Merchants Chongqing Communications Technology Research & Design Institute Co.,Ltd.
• Wei Zhang, Southwest University of Science and Technology
• Yugui Liu, Chongqing Jiaotong University
• Jianhui Xu, China Merchants Chongqing Communications Technology Research & Design Institute Co.,Ltd.
• Haidong Liu, Southwest University of Science and Technology
• Shutong Tang, China Merchants Chongqing Communications Technology Research & Design Institute Co.,Ltd.
• Junan Shen, Georgia Southern UniversityFollow

Document Type

Article

Publication Date

2-25-2026

Publication Title

Molecules

DOI

10.3390/molecules31050771

Abstract

The formation of recyclable polyethylene materials is significantly limited by traditional crosslinking methods, which involve solvent-heavy processes and permanent chemical bonds that cannot be undone. Herein, we report an environmentally friendly and scalable approach to construct a thermo-reversible polyethylene network (PE-g-DA) via solvent-free, one-step melt processing based on furan–maleimide Diels–Alder (D–A) dynamic covalent chemistry. Furan-functionalized polyethylene was dynamically crosslinked with bismaleimide during melt mixing, fully compatible with conventional polyolefin processing techniques. FTIR spectroscopy, temperature-dependent solubility, and differential scanning calorimetry collectively confirm the reversible formation and dissociation of D–A adducts, enabling thermal switching of the network structure. Equilibrium swelling experiments based on the Flory–Rehner model indicate that the crosslink density can be precisely controlled by varying the bismaleimide content. As a result, PE-g-DA exhibits significantly enhanced tensile strength while maintaining high ductility at moderate crosslink densities. Notably, the dynamic network allows efficient thermal reprocessing, with recycled samples retaining approximately 93% and 80% of their original tensile strength after the first and second reprocessing cycles, respectively. Moreover, intrinsic thermal self-healing behavior is directly visualized by scanning electron microscopy at 120 °C. This work demonstrates that combining dynamic Diels–Alder chemistry with solvent-free melt processing offers a practical and sustainable route to recyclable, reprocessable, and self-healable polyethylene materials with clear potential for large-scale industrial production.

Comments

Georgia Southern University faculty member, Junan Shen co-authored, "Thermally Reversible and Recyclable Polyethylene Networks via Furan–Maleimide Diels–Alder Dynamic Covalent Chemistry."

Recommended Citation

Hao, Zengheng, Wei Zhang, Yugui Liu, Jianhui Xu, Haidong Liu, Shutong Tang, Junan Shen. 2026. "Thermally Reversible and Recyclable Polyethylene Networks via Furan–Maleimide Diels–Alder Dynamic Covalent Chemistry." Molecules, 31 (5): MDPI. doi: 10.3390/molecules31050771
https://digitalcommons.georgiasouthern.edu/civil-eng-facpubs/189

Creative Commons License

This work is licensed under a Creative Commons Attribution 4.0 License.