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Peer-reviewedCC BYScience Advances

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

  • Eliza K. Neidhart1,2
  • Stephanie M. Ribet3,4
  • Taehyun A. Lee1,2
  • Logan T. Kearney5,6
  • Karen C. Bustillo3,4
  • Eric A. Dailing7,4
  • Mutian Hua8,7,9
  • Colin Ophus10,2
  • Sophia N. Fricke11,2
  • Ah-Young Song12,4
  • Jeffrey A. Reimer11,2
  • Erik J. Alexanian1
3 more authors
  • Joanna M. Atkin1
  • Brett A. Helms13,7
  • Frank A. Leibfarth1
13 affiliations
  1. 1Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, NC 27599, USA
  2. 2University of North Carolina at Chapel Hill
  3. 3National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA
  4. 4Lawrence Berkeley National Laboratory
  5. 5Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN 37830, USA
  6. 6Oak Ridge National Laboratory
  7. 7The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA
  8. 8School of Environmental and Forest Sciences, University of Washington, Seattle, WA 98195, USA
  9. 9Stanford University
  10. 10Department of Materials Science and Engineering, Stanford University, Stanford, CA 94305, USA
  11. 11Department of Chemical and Biomolecular Engineering, University of California Berkeley, Berkeley, CA 94720, USA
  12. 12College of Chemistry Pines Magnetic Resonance Center, University of California Berkeley, Berkeley, CA 94720, USA
  13. 13Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA
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Abstract

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.

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Cite

BibTeXRIS
BibTeX
@article{neidhart2026polyolefin,
  title = {{Polyolefin blends with co-continuous architectures enabled by dynamic covalent crosslinking}},
  author = {Eliza K. Neidhart and Stephanie M. Ribet and Taehyun A. Lee and Logan T. Kearney and Karen C. Bustillo and Eric A. Dailing and Mutian Hua and Colin Ophus and Sophia N. Fricke and Ah-Young Song and Jeffrey A. Reimer and Erik J. Alexanian and Joanna M. Atkin and Brett A. Helms and Frank A. Leibfarth},
  journal = {Science Advances},
  year = {2026},
  month = may,
  doi = {10.1126/sciadv.aee2328},
  url = {https://doi.org/10.1126/sciadv.aee2328},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Polyolefin blends with co-continuous architectures enabled by dynamic covalent crosslinking
AU  - Eliza K. Neidhart
AU  - Stephanie M. Ribet
AU  - Taehyun A. Lee
AU  - Logan T. Kearney
AU  - Karen C. Bustillo
AU  - Eric A. Dailing
AU  - Mutian Hua
AU  - Colin Ophus
AU  - Sophia N. Fricke
AU  - Ah-Young Song
AU  - Jeffrey A. Reimer
AU  - Erik J. Alexanian
AU  - Joanna M. Atkin
AU  - Brett A. Helms
AU  - Frank A. Leibfarth
PY  - 2026
DA  - 2026/05/15
JO  - Science Advances
DO  - 10.1126/sciadv.aee2328
UR  - https://doi.org/10.1126/sciadv.aee2328
AB  - 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.
SN  - 2375-2548
ER  -